Materials Science & Engineering R 146 (2021) 100644

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Materials Science & Engineering R

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High-entropy ceramics: Review of principles, production and applications

Saeid Akrami a, Parisa Edalati a, Masayoshi Fuji a, *, Kaveh Edalati b, *
a
Advanced Ceramics Research Center, Nagoya Institute of Technology, Tajimi, 507-0071, Japan
b
WPI, International Institute for Carbon-Neutral Energy Research (WPI-I2CNER), Kyushu University, Fukuoka, 819-0395, Japan

A R T I C L E I N F O A B S T R A C T

Keywords: High-entropy ceramics with five or more cations have recently attracted significant attention due to their su­
High-entropy alloys (HEAs) perior properties for various structural and functional applications. Although the multi-component ceramics have
Multi-principal element alloys been of interest for several decades, the concept of high-entropy ceramics was defined in 2004 by producing the
High-entropy ceramics
first high-entropy nitride films. Following the introduction of the entropy stabilization concept, significant efforts
Entropy stabilization
Functional properties
were started to increase the entropy, minimize the Gibbs free energy and achieve stable single-phase high-en­
Synthesis methods tropy ceramics. High-entropy oxides, nitrides, carbides, borides and hydrides are currently the most popular
high-entropy ceramics due to their potential for various applications, while the study of other ceramics, such as
silicides, sulfides, fluorides, phosphides, phosphates, oxynitrides, carbonitrides and borocarbonitrides, is also
growing fast. In this paper, the progress regarding high-entropy ceramics is reviewed from both experimental and
theoretical points of view. Different aspects including the history, principles, compositions, crystal structure,
theoretical/empirical design (via density functional theory, molecular dynamics simulation, machine learning,
CALPHAD and descriptors), production methods and properties are thoroughly reviewed. The paper specifically
attempts to answer how these materials with remarkable structures and properties can be used in future
applications.

1. Introduction (HENs), carbides (HECs), borides (HEBs), hydrides (HEHs), silicides

Entropy is a thermodynamic parameter which represents the degree
of anarchy or disorder in a material. Entropy is influenced by different
configurations, such as magnetic moment, atomic vibration and atomic
arrangement, while the latter one is usually the most effective config­
uration regarding entropy changes. Entropy has not been considered as
effective as enthalpy for material design until recent years, when the
concept of high-entropy alloys (HEAs) was introduced [1,2]. In 2004
and following some earlier ground studies, the concept of HEAs was
introduced by the parallel studies of Yeh et al. [1] and Cantor et al. [2],
who introduced a novel family of multi-component alloys. The HEAs are
usually defined as multi-principal element alloys (MPEAs) with a high
configuration entropy which are formed from five or more elements
with equal or close to equal atomic fractions [1]. These alloys exhibit a
unique combination of composition, microstructure and properties
[3–30]. Similar to HEAs, high-entropy ceramics are defined as the solid
solution of five or more cations or anions sublattices with a high
configuration entropy [31]. The high-entropy ceramics now include a
wide range of materials including high-entropy oxides (HEOs), nitrides
(HESis), sulfides (HESs), fluorides (HEFs) phosphides (HEPs), phos­
phates (HEPO4s), oxynitrides (HEONs), carbonitrides (HECNs) and
borocarbonitrides (HEBCNs).
In this paper, the development in the new field of high-entropy ce­
ramics is reviewed with a special attention on principles, historical and
publication trends, crystal structure, theoretical/empirical design, pro­
duction methods, properties and potential applications. Moreover, a
summary of publications in this field are given in the Appendix.
2. Principles
Stability of an elemental mixture in the form of a solid solution is
related to the Gibbs free energy changes (ΔGmix).
ΔGmix = ΔHmix − TΔSmix (1)
where ΔHmix is the enthalpy of the mixture, T is the absolute tempera­
ture and ΔSmix is the entropy of mixing. When the mixing entropy in­
creases, the Gibbs free energy decreases and the solid solution becomes
more stable [32,33]. The entropy is influenced by the temperature,

* Corresponding authors.
E-mail addresses: fuji@nitech.ac.jp (M. Fuji), kaveh.edalati@kyudai.jp (K. Edalati).

https://doi.org/10.1016/j.mser.2021.100644
Received 17 March 2021; Received in revised form 18 August 2021; Accepted 19 September 2021
Available online 7 October 2021
0927-796X/© 2021 Elsevier B.V. All rights reserved.
S. Akrami et al.
Fig. 1. Relation between entropy of mixing and number of elements and
definition of medium-entropy ceramics and high-entropy ceramics.
Fig. 2. Terminology of compositionally-complex ceramics or multi-principal
cation ceramics, suggested to cover a wide range of multi-component ce­
ramics including high-entropy ceramics [39].
number of elements and atomic fraction of each element in the
composition. The relationship between the atomic fraction of elements
and entropy of mixing is shown by the following equation.
∑
i=1
ΔSmix = − R xi lnxi (2)
N
In this equation, R is the gas constant, xi is the atomic fraction of ith
element and N is the total number of elements. Based on this equation,
the entropy of mixing for a specified number of elements reaches a
maximum value when the number of elements is high and they have an
equal atomic fraction. For the mixtures with equiatomic compositions,
the entropy of mixing can be simply calculated by Eq. (3).
ΔSmix = Rln N (3)
Fig. 1 demonstrates the relation between the entropy of mixing and
the number of elements for an equiatomic mixture of elements calcu­
lated using Eq. (3). This figure suggests a practical approach to enhance
the entropy and stabilize the medium-entropy and high-entropy single-
phase materials by increasing the entropy. This entropy stabilization not
only produces a high phase stability, but also results in interesting
properties due to the co-contribution of elements through several phe­
nomena such as the cocktail effect (each element provides a particular
property to the system), valence electron distribution, lattice distortion
(due to differences in the atomic diameter of the elements) and sluggish
diffusion [1–30].
There are different definitions for high-entropy materials [25,34]: (i)
the presence of at least five elements with 5–35 at% in the composition,
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Materials Science & Engineering R 146 (2021) 100644
(ii) a mixing entropy higher than 1.5R [35], and (iii) a mixing entropy
higher than 1.61R. It was suggested that when ΔSmix ≥ 1.5R, the high
amount of TΔSmix in Eq. (1) can overcome ΔHmix and make the Gibbs
free energy negative to produce a single phase. Although this concept is
totally correct at high temperatures, many multi-component alloys with
ΔSmix ≥ 1.5R are metastable or they have multiple phases at room
temperature due to the enthalpy effects [4,32,36,37].
Several issues should be considered regarding the terminology of
high-entropy ceramics [4,5,10,15,32,36,38]. First, high-entropy ce­
ramics should be principally single phase, but dual phase high-entropy
ceramics are recently included in this family of materials. Second, the
term “high-entropy” is rather paradoxical for ceramics because most of
these materials have ordered structures (they still have a higher entropy
compared to conventional ordered ceramics). Third, in most research
studies of multi-component systems, the term high entropy is used to
remind the large number of principal elements. Fourth, entropy stabi­
lization can occur not only in high-entropy ceramics (ΔSmix ≥ 1.5R, as
defined in Fig. 1), but also in medium-entropy ceramics (compositions of
3 or 4 cations with R ≤ ΔSmix < 1.5R, as defined in Fig. 1) and in some
other multi-component ceramics.
To address all these terminological inconsistencies, Wright et al. [39,
40] suggested that using the concept of compositionally-complex ce­
ramics or multi-principal cation ceramics can more appropriately cover
all these ceramics. They suggested that compositionally-complex ce­
ramics consist of high-entropy ceramics with equiatomic or near
equiatomic compositions, entropy-stabilized ceramics, medium-entropy
ceramics and non-equiatomic compositions (Fig. 2). The
entropy-stabilized ceramics refer to ceramics that their stability is
improved by enhancing the entropy through increasing the number of
principal elements, as described in section 2 [32,41]. The main focus of
the current review paper is on high-entropy ceramics with five or more
cations, but some other multi-principal cation ceramics are also
included.
3. Historical and publication trends
Fig. 3 is an image showing that there has been a continuous trend to
increase the number of elements in engineering materials since the start
of civilization: from bronze to cast iron, aluminum alloys, magnesium
alloys, amorphous alloys and currently to HEAs [42,43]. There have
been some scientific movements in this direction within centuries. The
German scientist, Karl Franz Achard, is one of the first people who tried
to fabricate alloys with up to seven principal elements. His work, which
was published in 1788, was appreciated decades later by Smith in 1963
[44]. In another important scientific movement, Greer’s confusion
principle suggested that increasing the number of elements in alloys
should lead to increasing the chaotic entropy and ability to form an
amorphous structure [45]. Greer’s confusion principle was examined
later by Cantor et al., who performed induction melting and melt
quenching on an equiatomic mixture of 20 elements (Mn, Cr, Fe, Co, Ni,
Cu, Ag, W, Mo, Nb, Al, Cd, Sn, Bi, Pb, Zn, Ge, Si, Sb and Mg) and 16
elements (Mn, Cr, Fe, Co, Ni, Cu, Ag, W, Mo, Nb, Al, Cd, Sn, Pb, Zn and
Mg), but they ended with polycrystalline materials despite the high
number of elements [45–47]. There were some other ground studies in
the field of high-entropy materials from 1970 to 2003 [1,2,29,36,
48–53], but the concept of HEAs was clearly introduced in 2004 [1,2].
Within the history of civilization, the number of elements in ceramics
has been usually higher than that in alloys due to the presence of various
multi-component ceramics such as clay in nature. There have been
extensive attempts, particularly within the last century, to produce less
complicated binary or ternary ceramics from these complex natural
ceramics and use them for various engineering applications. However, a
search in Scopus shows that there have been some scientific activities
regarding multi-component ceramics since 1964, although none of these
publications clearly introduced the concept of entropy stabilization until
2004–2005 [48,54]. The introduction of high-entropy ceramics in
 S. Akrami et al. Materials Science & Engineering R 146 (2021) 100644

Fig. 3. Schematic illustration of engineering materials development within history, showing the continuous trend to increase entropy [43].

about HEOs had a slow growth. In 2015, the concept of

Fig. 4. Number of publications per year about main high-entropy ceramics
including oxides, nitrides, carbides, borides and hydrides. This figure was
plotted based on the data searched in Scopus on August 12, 2021 (total number
of publications: 477).
2004–2005 was an extension of the concept of metallic HEAs to ceramics
by including both metallic and non-metallic elements [55].
Fig. 4 shows the number of publications per year for main high-
entropy ceramics including HEOs, HENs, HECs, HEBs and HEHs. Pub­
lications about high-entropy ceramics gradually appeared after
2004–2005 but experienced a significant growth in 2019–2021. It is
assumed that the number of publications in 2020 and 2021 was nega­
tively influenced by the spread of the COVID-19 virus all over the world.
A brief review of the publication trends is given below.
In 2004, Chen et al. [48] fabricated nitrides of Fe-Co-Ni-Cr-Cu-Al-Mn
and Fe-Co-Ni-Cr-Cu-Al0.5 by reactive DC sputtering and investigated the
mechanical properties. They continued their study in 2005 by
comparing the nitrides of AlxCoCrCuFeNi and AlCrNiSiTi and showed
that the hardness of the latter nitride is much higher than the former one
[54]. As shown in Fig. 3, after 2005, the number of publications about
HENs slowly increased for almost one decade, but the number has
significantly increased in recent years due to the popularity of
high-entropy materials.
Following the introduction of HENs, the second kind of high-entropy
ceramics as HEOs, was introduced in 2007 by Chen et al. [56]. They
produced thin film oxides of AlxCoCrCuFeNi (x = 0.5, 1, 2) and inves­
tigated their hardness and bandgap in 2007 [56] and their thermal
stability in 2008 [57]. From 2007 to 2015, the number of publications
high-entropy-stabilized ceramics was highlighted by Rost et al. [58],
who could stabilize HEOs with a single rock-salt phase and five different
cations in equiatomic fractions. This publication can be considered as
another turning point in the field of high-entropy ceramics which led to
a significant increase in the number of publications about HEOs.
Currently, the highest number of publications about high-entropy ce­
ramics is related to HEOs due to their interesting scientific aspects,
specific properties and potential applications such as thermal properties,
catalysis, ionic conductivity, magnetic properties, electrical properties,
etc.
HECs were introduced in 2010 by Braic et al. [59] by fabrication of
(TiAlCrNbY)C films by reactive magnetron sputtering. In 2011 Chang et al.
[60] combined HECs with HENs and introduced (AlCrTaTiZr)NxCy as an
HECN. The publication numbers about HECs reached a high level in 2019
and 2020, making them the second most popular high-entropy ceramics.
HEBs were mainly introduced in 2016 by Gild et al. [61], who introduced
(Hf0.2Zr0.2Ta0.2Cr0.2Ti0.2)B2, (Mo0.2Zr0.2Ta0.2Nb0.2Ti0.2)B2, (Hf0.2Mo0.2
Ta0.2Nb0.2Ti0.2)B2, (Hf0.2Zr0.2Mo0.2Nb0.2Ti0.2)B2, (Hf0.2Zr0.2Ta0.2Mo0.2Ti0.2)
B2 and (Hf0.2Zr0.2Ta0.2Nb0.2Ti0.2)B2 as ultrahigh-temperature ceramics.
There have been some interests about multi-component hydrides
even from 2000 for hydrogen storage application [62]. However, the
application of HEHs for hydrogen storage was clearly discussed in a
publication in 2010 [63]. For other high-entropy ceramics, there have
been rather limited studies in the literature which were mainly pub­
lished in recent years: HESis in 2019–2020 [64–68], HESs in 2018 [69],
HEFs in 2020 [70,71], HEPs in 2020 [72], HEPO4s in 2019 [73], HEONs
in 2018 [74], HECNs in 2011 [60] and HEBCNs in 2020 [75] and
high-entropy cermets in 2017 [76].
4. Crystal structures
The crystal structures of high-entropy ceramics have a significant
effect on their properties. In this section, the crystal structure of HEOs is
first discussed due to the significant information reported about these
ceramics. The crystal structures of other ceramics are explained alto­
gether in the second subsection. The main crystal structures of the high-
entropy ceramics are summarized in Table 1.
4.1. Crystal structure of high-entropy oxides
The rock-salt, fluorite, perovskite, pyrochlore and spinel phases are
the most typical crystal structures of the HEOs. Within the past several
years, some reasonable correlations between the composition, synthesis

3
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S. Akrami et al. Materials Science & Engineering R 146 (2021) 100644

Table 1
Main crystal structures of the high-entropy ceramics.
Structure Crystallography Appearance Reference

High-Entropy Oxide (HEOs)

Rock-salt Cubic (Fm-3 m) [77]

Fluorite A2B2O7 cubic (Fm-3 m) [78]

Perovskite ABO3 Orthorhombic (Pbnm) [79]

Perovskite ABO3 Cubic (Pm3 m) [80]

Perovskite ABO3 Hexagonal (P63/mmc) [81]

Spinel AB2O4 Cubic (Fd-3 m) [82]

Pyrochlore A2B2O7 Cubic (Fd-3 m) [83]

High-Entropy Nitrides (HENs)

NaCl-type Cubic (Fm-3 m) [84]
(continued on next page)

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S. Akrami et al. Materials Science & Engineering R 146 (2021) 100644

Table 1 (continued )
Structure Crystallography Appearance Reference

High-Entropy Carbides (HECs)

Rock-salt (NaCl-type) Cubic (Fm-3 m) [85]

High-Entropy Borides (HEBs)

AlB2 Hexagonal (P6/mmm) [86]

High-Entropy Silicides (HESis)

CrSi2 prototype Hexagonal (P6222) [64]

High-Entropy Fluorides (HEFs)

Perovskite ABF3 Cubic (Pm3 m) [71]

High-Entropy Phosphates (HEPO4)

Monazite-type Monoclinic (P21/n) [73]

methods, properties and crystal structure of HEOs were established.
Here, the main focus is on the compositional characteristics of each
crystal structure, but the synthesis method and main properties of each
structure are briefly mentioned. Details of the synthesis method and
properties are separately reviewed in this paper.
4.1.1. Rock-salt structure
The cubic rock-salt structure can be observed in various oxides
including HEOs. Most of the HEOs with the rock-salt structure are based
on Mg-Co-Ni-Cu-Zn. These oxides can be fabricated by various synthesis
methods such as the solid-state reaction [58,86–100], nebulized spray
pyrolysis [101–105], flash-assisted synthesis [106], reaction-assisted
flash sintering [107], polymeric synthesis route [108], co-precipitation
and hydrothermal synthesis [109], solution combustion [110,111] and
pulsed-laser deposition [112]. The rock-salt Mg-Co-Ni-Cu-Zn-O ce­
ramics are of interest from different points of view such as Li conduc­
tivity [92,96,97,101,104,113,114], structural features [58,89–91,93,
99,102,103,106,107,111,112,115], catalysis [94], magnetic properties
[77,98,110,116], electrical properties [88,95], thermal properties [109]
and mechanical properties [100]. The HEOs with the rock-salt structure
demonstrate high dielectric constants [88] and superionic conductivity
[113] which make these materials attractive for future applications as
large-k dielectric materials and solid-state electrolytes for batteries.
In one of the earliest attempts to produce the rock-salt HEOs, Rost

5
S. Akrami et al.
Table 2
Chemical composition of high-entropy oxides with fluorite crystal structure.
(Ce0.2La0.2Pr0.2Sm0.2Y0.2)O2-δ [102], (Hf0.25Zr0.25Ce0.25Y0.25)O2-δ [118],
(Hf0.25Zr0.25Ce0.25) (Y0.125Yb0.125)O2-δ [118], (Hf0.2Zr0.2Ce0.2)(Y0.2Yb0.2)O2-δ [118],
(Hf0.25Zr0.25Ce0.25)(Y0.125Ca0.125)O2-δ [118], (Hf0.2Zr0.2Ce0.2)(Y0.2Gd0.2)O2-δ [118],
(Hf0.25Zr0.25Ce0.25)(Y0.125Gd0.125)O2-δ [118], (Hf0.25Zr0.25Ce0.25)(Yb0.125Gd0.125)
O2-δ [118], (Hf0.2Zr0.2Ce0.2)(Yb0.2Gd0.2)O2-δ [118], Ce0.2Zr0.2Y0.2Gd0.2La0.2O2− δ
[120], (Y0.25Yb0.25Er0.25Lu0.25)2(Zr0.5Hf0.5)2O7 [78],
(Hf1/3Zr1/3Ce1/3)1-x(Y1/2X1/2)xO2-δ (X = Yb, Ca, Gd; x = 0.4, 0.148, 0.058) [39],
(Sc0.2Ce0.2Pr0.2Gd0.2Ho0.2)2O3±δ [121], (Ce,Gd,Nd,Sm,Pr,Mox)O2-δ [119], (Ce,Gd,
La,Nd,Pr,Mox)O2-δ [119]
et al. [58] introduced (Mg0.2Co0.2Ni0.2Cu0.2Zn0.2)O and examined the
concept of entropy stabilization for this oxide. The reason to choose this
system was the variety of structures, coordination and atomic radius of
the mono oxides [77]. Rost et al. investigated the homogeneity and local
structure of the rock-salt structure in these HEOs by the X-ray absorption
fine structure method [90]. Their results showed that the local
metal-oxygen bond length is different around each cation, but the
interatomic distances were uniform for the cation-cation pairs.
Furthermore, they showed that the crystal models fit with the experi­
mental scattering data for the rock-salt structure. They reported that the
cations are randomly distributed on an Fm-3 m sublattice with minor
local disorder. They also found an interleaved Fm-3 m anion sublattice
with oxygen ions dislocated from the ideal positions to make the dis­
tortions in the cation polyhedra [90].
Sarkar et al. [103] fabricated (Co,Mg,Ni,Zn)O and (Co,Cu,Mg,Ni,Zn)
O entropy-stabilized oxides with the rock-salt structure by three
different synthesis routes (nebulized spray pyrolysis, flame spray py­
rolysis and reverse co-precipitation) and demonstrated that the crystal
structures of these materials do not depend on the synthesis method. The
rock-salt phase was directly achieved after nebulized spray pyrolysis,
while a heat treatment was necessary to stabilize the rock-salt phase
after synthesis by flame spray pyrolysis and reverse co-precipitation.
Brardan et al. [89] studied the effect of the synthesis conditions,
stoichiometry and annealing on the structure of the rock-salt MgCoNi­
CuZnO-based HEOs. They confirmed the important role of Cu in the
crystal structure. They found that the shape, width and intensity of the
Bragg peaks deviate from the ideal mode for the rock-salt structure by
increasing the Cu concentration. They attributed these behaviors to
evolution of the local environment of the Cu2+ ions from octahedral in
the Cu-poor materials to rhombic in the Cu-rich samples.
Dupuy et al. [93] investigated the effect of the grain size on the phase
transformation of the (Co,Cu,Mg,Ni,Zn)O rock-salt oxide. They found
that small grain sizes lead to increasing the amount of a secondary
Cu-rich tenorite phase and decreasing the phase transformation
temperature.
Grzesik et al. [99] investigated the phase transformation, defect
structure and chemical diffusion of the rock-salt (Co,Cu,Mg,Ni,Zn)O at
the temperature of 1173 K under various oxygen pressures of 10− 105
Pa. No phase transformations occurred in the investigated ranges of
temperature and oxygen pressure, but large fractions of anion vacancies
were detected in the rock-salt phase. They found a non-logarithmic
dependence of the diffusivity on the pressure, suggesting that the
interacting defects have a complex structure compared to the conven­
tional rock-salt phases.
Chen et al. [91] studied the effect of Li and Mn doping on the stability
of the rock-salt phase in MgCoNiCuZnO5 under high pressures and
temperatures. Their results showed that the rock-salt phase is stable at
temperatures up to 723 K and pressures up to ~50 GPa. The Li and Mn
doping made the HEO more compressible due to the presence of weak
Li–O and MnO– bonds, confirming the importance of doping on the
mechanical properties and ion conductivity of the rock-salt HEOs. Car­
doso et al. [117] also showed that the Gd doping is effective to control
the lattice expansion and asymmetry of the rock-salt phase.
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Materials Science & Engineering R 146 (2021) 100644
4.1.2. Fluorite structure
Table 2 shows the chemical composition of the HEOs with the cubic
fluorite crystal structure. These HEOs are fabricated by different syn­
thesis routes such as nebulized spray pyrolysis [102], ball milling and
spark plasma sintering [39,78,118,119] co-precipitation and hydro­
thermal treatment [120,121]. The structural features [102], thermal
behavior [39,78,118,120] and mechanical properties [39] of these
materials were their main investigated features.
Following the introduction of entropy-stabilized rock-salt oxides
[122], many researchers attempted to extend this theoretical concept to
other oxides such as rare-earth and transition-metal oxides with
different crystal structures including the cubic fluorite structure [120].
Due to the functional properties of the rare-earth oxides with the fluorite
structure [123–126], their synthesis with the high-entropy features was
one of the main attempts. There are now some rules for fabricating the
rare-earth-based HEOs with the fluorite structure: i) the radius of all the
cations should be similar, ii) at least one cation oxide should have a
different crystal type, and iii) at least one cation does not have any
miscibility on the binary phase diagram [127]. Sarkar et al. [128]
showed that the Ce4+ presence is necessary to stabilize the
rare-earth-based HEOs with the fluorite structure.
There are also a few general formulations for the high-entropy
fluorite oxides. The most famous ones are (CeRE)O2− δ and (HfZrCeM)
O2− δ, in which RE stands for the rare-earth elements, such as La, Ce, Y,
Yb, etc, M stands for other metals and δ depends on the cation valence
[129]. There is another formulation in the form of RE2TM2O7, in which
TM stands for the transition metals and particularly for Ti, Zr and Hf.
The structure of these components is determined by the ratio of the RE
cation radius to TM cation radius. If the ratios are in the range of
1.46–1.78, the component shows a pyrochlore structure; however, when
the ratio is 1.46, the component shows a fluorite structure [78].
RE2TM2O7 high-entropy oxides can be used as environmental/thermal
barrier coatings due to their low thermal conductivity, high thermal
stability and their tunable thermal expansion coefficients [130–134].
Wright et al. [39] showed that the addition of the Ca2+ cation to fluorites
can create O2− oxygen vacancies with a concentration two times higher
than those produced by the 3+ cations. They commented that due to the
positive effect of oxygen vacancies on the fluorite phase formation [39,
135], the stability of fluorite in HEOs with the Ca2+ cations should be
due to the formation of additional oxygen vacancies [39].
4.1.3. Perovskite structure
HEOs with the perovskite structure are another popular group of
high-entropy ceramics which are synthesized by methods such as
nebulized spray pyrolysis [79,102,136,137], solid-solistate reaction and
sintering [138–141], reactive spark plasma sintering [142],
sonochemical-based synthesis [80], molten salt method [143], flash
sintering [144,145], pulsed laser deposition [146] and co-precipitation
[147]. These high-entropy perovskite oxides were investigated for their
properties and applications such as dielectric and electrical properties
[138,141,143,145,146,148–151], magnetic properties [79,152], ther­
mal properties [147], ion conductivity [153], sintering behavior [142,
144] and catalysis [80].
Table 2 summarizes the chemical composition of the HEOs with the
perovskite crystal structure. These perovskites, having either cubic,
orthorhombic or hexagonal crystal structure, should contain at least two
cation sublattices in the form of ABO3, in which A and B show two types
of different cation groups [139]. The ABO3-type perovskite structure
consists of B-type cations in a 6-fold coordination, A-type cations in a
12-fold coordination and an octahedral oxygen anion [139]. The ability
of perovskites to show some interesting properties is due to their
chemical and structural features, which can place cations with different
properties in two cationic subsets [140]. The stability of the perovskite
structure can be predicted by the Goldschmid tolerance factor, tG [154].
S. Akrami et al.
Table 3
Chemical composition of high-entropy oxides with perovskite crystal structure.
(Gd0.2La0.2Nd0.2Sm0.2Y0.2)CoO3 [136,137], (Gd0.2La0.2Nd0.2Sm0.2Y0.2)CrO3 [136,
137], (Gd0.2La0.2Nd0.2Sm0.2Y0.2)FeO3 [136,137], (Gd0.2La0.2Nd0.2Sm0.2Y0.2)MnO3
[136], (Gd0.2La0.2Nd0.2Sm0.2Y0.2)NiO3 [136], Gd(Co0.2Cr0.2Fe0.2Mn0.2Ni0.2)O3 [79,
136], La(Co0.2Cr0.2Fe0.2Mn0.2Ni0.2)O3 [79,136,152], Nd(Co0.2Cr0.2Fe0.2Mn0.2Ni0.2)
O3 [79,136], Sm(Co0.2Cr0.2Fe0.2Mn0.2Ni0.2)O3 [79,136], Y
(Co0.2Cr0.2Fe0.2Mn0.2Ni0.2)O3 [79,136], (Gd0.2La0.2Nd0.2Sm0.2Y0.2)
(Co0.2Cr0.2Fe0.2Mn0.2Ni0.2)O3 [79,102,136], BaO-SrO-CaO-MgO-PbO-TiO2 [141],
BaO-SrO-CaO-MgO-PbO-Fe2O3 [141], Na2O-K2O-CaO-La2O3-Ce2O3-TiO2 [141], Pb
(Zr0.49Ti0.51)0.94Mn0.014Sb0.02W0.014Ni0.02O3 [150], Sr(Zr0.2Sn0.2Ti0.2Hf0.2Mn0.2)O3
[139], Sr(Zr0.2Sn0.2Ti0.2Hf0.2Nb0.2)O3 [139], Ba(Zr0.2Sn0.2Ti0.2Hf0.2Ce0.2)O3 [139],
Ba(Zr0.2Sn0.2Ti0.2Hf0.2Y0.2)O3 [139], Ba(Zr0.2Sn0.2Ti0.2Hf0.2Nb0.2)O3 [139,140,
151], (Sr0.5Ba0.5)(Zr0.2Sn0.2Ti0.2Hf0.2Nb0.2)O3 [139],
(Bi1-x-yNa0.925-x-yLi0.075)0.5BaxSryTiO3 [138], Sr((Zr0.94Y0.06)0.2Sn0.2Ti0.2Hf0.2Mn0.2)
O3− x [142], Na0.30K0.07Ca0.24La0.18Ce0.21TiO3 [141], BaSr(ZrHfTi)O3 [80], BaSrBi
(ZrHfTiFe)O3 [80], Ru/BaSrBi(ZrHfTiFe)O3 [80],
Pb0.94Sr0.06(Zr0.50Ti0.50)0.99Cr0.01O3 [148], (Li0.06Na0.47K0.47)(Nb0.94Sb0.06)O3
[143], Ba(Zr0.2Ti0.2Sn0.2Hf0.2Ta0.2)O3 [151], Sr(Ti0.2Y0.2Zr0.2Sn0.2Hf0.2)O3-x [144],
(Na0.2Bi0.2Ba0.2Sr0.2Ca0.2)TiO3 [149], (La0.2Pr0.2Nd0.2Sm0.2Eu0.2)NiO3 [146], [(Bi,
Na)1/5(La,Li)1/5(Ce,K)1/ 5Ca1/5Sr1/5]TiO3 [153], (Y0.2Nd0.2Sm0.2Eu0.2Er0.2)AlO3
[147], (Bi0.2Na0.2K0.2Ba0.2Ca0.2)TiO3 [145]
Table 4
Chemical composition of high-entropy oxides with spinel crystal structure.
(Mg0.2Ti0.2Zn0.2Cu0.2Fe0.2)3O4 [156], (Co,Cu,Fe,Mn,Ni)3O4 [82], (Co,Cr,Fe,Mn,
Ni)3O4 [157,158,159,164], (Co,Cr,Fe,Mg,Mn)3O4 [157], (Cr,Fe,Mg,Mn,Ni)3O4
[157], (Cr0.2Fe0.2Mn0.2Ni0.2Zn0.2)3O4 [161], (Cr0.2Fe0.2Mn0.2Co0.2Zn0.2)3O4 [161],
(Co,Cr,Fe,Mg,Mn)3O4 [157], (Cr,Fe,Mg,Mn,Ni)3O4 [157],
(Al1/6Co1/6Cr1/6Fe1/6Mn1/6Ni1/6)3O4 [160],
NiFe1.9(Dy0.02Er0.02Gd0.02Ho0.02Tb0.02)O4 [163], (Co0.2Cr0.2Fe0.2Mn0.2Ni0.2)Fe2O4
[163], (Co0.2Cr0.2Fe0.2Mn0.2Ni0.2)Fe1.9(Dy0.02Er0.02Gd0.02Ho0.02Tb0.02)O4 [163],
AlxCoCrCuFeNi oxide [56,57], (Ni,Fe,Co,Cr,Al)Ox [162],
(Cr0.2Fe0.2Mn0.2Mg0.2Zn0.2)3O4 [111], (Co,Mg,Mn,Ni,Zn)(Al,Co,Cr,Fe,Mn)2O4
[173]
Table 5
Chemical composition of high-entropy oxides with pyrochlore crystal structure.
(Gd1/4Eu1/4Sm1/4Nd1/4)2Zr2O7 [174], (Gd1/5Eu1/5Sm1/5Nd1/5La1/5)2Zr2O7 [174],
(Gd1/6Eu1/6Sm1/6Nd1/6La1/6Dy1/6)2Zr2O7 [174],
(Gd1/7Eu1/7Sm1/7Nd1/7La1/7Dy1/7Ho1/7)2Zr2O7 [174],
(La0.2Nd0.2Sm0.2Eu0.2Gd0.2)2Zr2O7, (Y0.2Nd0.2Sm0.2Eu0.2Gd0.2)2Zr2O7,
(La0.2Y0.2Sm0.2Eu0.2Gd0.2)2Zr2O7 [83], (La0.2Nd0.2Y0.2Eu0.2Gd0.2)2Zr2O7 [83],
(La0.2Nd0.2Sm0.2Y0.2Gd0.2)2Zr2O7 [83], (La0.2Nd0.2Sm0.2Eu0.2Y0.2)2Zr2O7 [83],
(La0.2Ce0.2Nd0.2Sm0.2Eu0.2)2Zr2O7 [176], (La0.2Ce0.2Nd0.2Sm0.2Eu0.2)2Zr2O7 [177],
Sm2(Sn1/4Ti1/4Hf1/4Zr1/4)2O7 [175], Gd2(Sn1/4Ti1/4Hf1/4Zr1/4)2O7 [175],
(Sm1/2Gd1/2)2(Ti1/3Hf1/3Zr1/3)2O7 [175], (Eu1/2Gd1/2)2(Ti1/3Hf1/3Zr1/3)2O7 [175],
(La1/2Pr1/2)2(Sn1/3Hf1/3Zr1/3)2O7 [175], (Eu1/2Gd1/2)2(Sn1/3Hf1/3Zr1/3)2O7 [175],
(La1/3Pr1/3Nd1/3)2(Hf1/2Zr1/2)2O7 [175], (Sm1/3Eu1/3Gd1/3)2(Hf1/2Zr1/2)2O7 [175],
(Sm1/3Eu1/3Gd1/3)2(Sn1/3Hf1/3Zr1/3)2O7 [175],
(Sm1/3Eu1/3Gd1/3)2(Ti1/4Sn1/4Hf1/4Zr1/4)2O7 [175],
(Sm1/4Eu1/4Gd1/4Yb1/4)2(Ti1/4Sn1/4Hf1/4Zr1/4)2O7 [175],
(Sm1/3Eu1/3Gd1/3)2(Ti1/2Sn1/6Hf 1/6Zr1/6)2O7 [175],
(Sm1/3Eu1/3Gd1/3)2(Ti3/4Sn1/12Hf1/12Zr1/12)2O7 [175], (Sm1/3Eu1/3Gd1/3)2Ti2O7
[175], (Sm1/4Eu1/4Gd1/4Yb1/4)2(Ti1/2Hf1/4Zr1/4)2O7 [175],
(Sm3/4Yb1/4)2(Ti1/2Zr1/2)2O7 [175], (La1/5Ce1/5Nd1/5Sm1/5Eu1/5)2Zr2O7 [175],
(La1/7Ce1/7Pr1/7Nd1/7Sm1/7Eu1/7Gd1/7)2(Hf1/2Zr1/2)2O7 [175],
(La1/7Ce1/7Pr1/7Nd1/7Sm1/7Eu1/7Gd1/7)2(Sn1/3Hf1/3Zr1/3)2O7 [175]
RA + RO
tG = √̅̅̅
2 (RB + RO )
where RA , RB and RO refer to the radius of the A cations, B cations and
oxygen anion, respectively.
The perovskite structure is stable when 0.75 ≤ tG ≤1: when tG ~ 1, a
cubic phase is formed; and when tG < 1, other perovskite structures are
formed [155]. There are two general formulations for high-entropy
perovskites. The first formulation is (SrBa)(M)O3 in which M refers to
metals and the second one is (RE)(TM)O3 in which RE and TM refer to
the rare-earth elements and the transition metals, respectively [129]
(Table 3).
Materials Science & Engineering R 146 (2021) 100644
Sarkar et al. [136] investigated 11 (RE)(TM)O3-type HEOs (10 with
six cations and one with 10 cations) in terms of the perovskite phase
stability. Their results showed that seven HEOs including the 10-cation
oxide have a single-phase perovskite structure with a homogeneous and
random distribution of cations due to the high-entropy effect. The
reason for the instability of the perovskite phase in four other systems
was attributed to the enthalpy effect that could overcome the entropy
stabilization.
Chellali et al. [102] investigated three types of HEOs in terms of the
homogeneous distribution of elements on the atomic scale by atom
probe tomography. They synthesized the HEOs by nebulized spray py­
rolysis and compacted them under 6 GPa. They showed that even after
compression, the perovskite phase is stable and has a homogeneous
elemental distribution.
Vinnik et al. [141] investigated the formation of single-phase
high-entropy perovskite oxides using sintering. They synthesized
BaO-SrO-CaO-MgO-PbO-TiO2, BaO-SrO-CaO-MgO-PbO-Fe2O3 and
Na2O-K2O-CaO-La2O3-Ce2O3-TiO2 oxides and examined the significance
of the sintering temperature on the crystal structure. They showed that
the optimum sintering temperature to achieve a single-phase perovskite
structure is between 1423 and 1673 K [141].
4.1.4. Spinel structure
Spinels with the Fd-3 m cubic structure are another major group of
HEOs which are synthesized by different routes including the solid-state
reaction [156–158], solvothermal synthesis [82], solution combustion
synthesis [111,159–161], sol-gel auto-combustion [162,163] and reac­
tive sputtering [56,57]. HEOs with the spinel structure were investi­
gated for a wide range of properties and applications including ion
conductivity [156], catalysis [82,162], thermal, electrical and me­
chanical properties [56,57,157,158], structural properties [111,164,
165] and particularly the magnetic properties [159–161,163,165–167].
Table 4 summarizes the composition of the spinel HEOs. Spinel-type
magnetic oxides or ferrites have the general formulation of AB2O4, in
which the A cations are divalent, such as Mg, Zn, Mn and Co, and the B
cations are trivalent such as Fe, Cr and Al [168–170]. The addition of
Al3+ to the spinel ferrites is an effective strategy to control the magnetic
properties [171,172].
The production of single-phase spinels has been a challenging issue,
but there is now important information leading to the selection of the
best compositions and processes to produce the spinel structure. In one
of the first attempts, Rost et al. [122] did not succeed in producing a
single-phase spinel; however, Dąbrowa et al. [164] succeeded later in
synthesizing (Co,Cr,Fe,Mn,Ni)3O4 with a single spinel phase. Stygar
et al. [157] examined the effect of the composition on the formation of
the spinel phase in the Co-Cr-Fe-Mg-Mn-Ni-O system and showed that
Co-Cr-Fe-Mg-Mn-Ni-O, Co-Fe-Mg-Mn-Ni-O, Co-Cr-Fe-Mg-Ni-O and
Co-Cr-Mg-Mn-Ni-O consist of dual rock-salt and spinel phases, and
Co-Cr-Fe-Mn-Ni-O, Cr-Fe-Mg-Mn-Ni-O and Co-Cr-Fe-Mg-Mn-O consist of
a single spinel phase. They also reported that the sintering temperature
should be selected carefully because there is a tendency for the phase
transformation from the spinel phase to the rock-salt phase by sintering
at 1173− 1373 K. They demonstrated that there is an undesirable trend
for the separation of Mg and Ni from the spinel HEOs, but such a trend is
less for Fe and Cr. Fracchia et al. [173] could successfully produce an
(4)
eight-cation spinel (Co,Mg,Mn,Ni,Zn)(Al,Co,Cr,Fe,Mn)2O4 with a high
entropy on the tetrahedral and octahedral A and B cation sites, sug­
gesting new ferrites can be made from spinel HEOs [173].
4.1.5. Pyrochlore structure
HEOs with the pyrochlore structure, which are usually synthesized
by a solid-state reaction [83,174,175] and co-precipitation [176,177],
were investigated in terms of its structural features [174], mechanical
properties [83,175–177] and thermal conductivity [81,175–177].
Table 5 gives the chemical composition of the pyrochlore HEOs. These
oxides are an important class of structural/functional ceramics with two
7
S. Akrami et al.
types of A and B cations in the form of A2B2O7. Since the A cations are
usually rare-earth (RE) elements and the B cations are transition metals
(TM), the general formulation of the pyrochlores can be denoted as
(RE)2(TM)2O7. The A-type cations with a large atomic size are coordi­
nated with two 8b oxygen ions and six 48ƒ oxygen ions. The B-type
cations, which are smaller, are coordinated to six oxygen ions located on
48ƒ. An oxygen vacancy is located at 8a that is surrounded by four B
cations [174]. Another general formulation for pyrochlores is given as
(RE)2Zr2O7, which are known as rare-earth zirconates. Since rare-earth
zirconates with the pyrochlore structure have an ordered fluorite-type
structure with two cationic sublattices, they are considered as alterna­
tives for the yttria-stabilized zirconia for thermal barrier coatings
[178–180] with a high elastic modulus [181–183] and low thermal
conductivity [184–187]. A main research objectives of the pyrochlore
HEOs is reducing the heat conductivity using other rare-earth elements
on the A site [188–194] or B site [189,194].
4.1.6. Other oxide structures
Bixbyite [195], rutile [196], monoclinic [197–199], magneto­
plumbite [200], amorphous [201–207], face-centered cubic (FCC)
[208–210] and CaF2-type crystals [111,211] are the other reported
structures for the HEOs. These structures are sometimes more distorted
than similar structures in binary or ternary oxides, but they can have a
better phase stability. For example, the HEO lanthanide sesquioxide,
Gd0.4Tb0.4Dy0.4Ho0.4Er0.4O3, synthesized by Tseng et al. [195] has a
cubic-bixbyite structure within a wide range of temperatures up to 1923
K. Such a phase stability is better than the monocationic sesquioxides,
such as Gd2O3 and Tb2O3, which suffer from undesirable
temperature-induced phase transformations and deterioration of their
magnetic and dielectric properties. There are some other crystal struc­
tures for HEOs which are summarized in Table A1 of the Appendix.
4.2. Crystal structure of other ceramics
HENs are formed either with the amorphous or crystalline structure.
When the nitrogen activity in the synthesis process is sufficient, a
crystalline structure can be stabilized [84]. Most of the HENs with the
solid-solution crystalline form have the FCC (NaCl-type) structure [84].
The general formulation for the HENs is (TM)(PE)N in which TM stands
for the transition metals with the ability to form a nitride (Y, Ti, Zr, V,
Nb, Cr, Mo, Mn, Fe, Ru, Co, Ni and Cu) and PE stands for the elements
with the p orbital which can undergo covalent bonding with the nitrogen
(Al, Si, C and B) [84].
Carbides and borides mostly form an FCC rock-salt structure or an
AlB2-type hexagonal structure containing layers of two-dimensional
carbide/borides and cations. Most of the carbides and borides follow
the formulations (TM)C and (TM)B2 (high-entropy diboride), although
the HEBs with the formulation of (RE)B6 (high-entropy hexaboride) can
also be synthesized [212].
There is a reversible process between the HEAs and their HEHs. The
alloys usually have the body center cubic (BCC) and C14-type Laves
phase structures [63,213–217]. HEHs can have different structures
including the FCC, base-centered tetragonal (BCT) and C14 Laves
structure. The Laves phase usually shows the lowest thermodynamic
stability for hydrogen release and BCT shows a high stability [213–215,
217–227].
HESis usually have a hexagonal or cubic structure. It was reported
that (Mo0.2W0.2Cr0.2Ta0.2Nb0.2)Si2 and (Mo0.2Nb0.2Ta0.2Ti0.2W0.2)Si2
[64] have a C40-type hexagonal structure [67], (TiZrNbMoW)Si2 [68]
and (Ti0.2Zr0.2Nb0.2Mo0.2W0.2)Si2 [65] have the hexagonal closed
packed (HCP) structure, and (Mo0.25Nb0.25Ta0.25V0.25)(Al0.5Si0.5)2
alumino-silicide has the CsCl-type B2 structure [66].
The investigation of the crystal structures of the HESs is quite
limited. It was reported that the HESs, Cu5SnMgGeZnS9 and Cu3SnM­
gInZnS7, produced by ball milling and spark plasma sintering have the
tetragonal structure [69].
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Materials Science & Engineering R 146 (2021) 100644
There are two main types of crystal structures for the HEFs: fluorite
and perovskite. CeNdCaSrBaF12 is among the HEFs with the fluorite
structure [70] and K(MgMnFeCoNi)F3, K(MgMnCoNiZn)F3, K(MnFeCo­
NiZn)F3 and K(MgCoNiCuZn)F3 are among the HEFs with the perovskite
structure [71].
HEP (Co,Cr,Fe,Mn,Ni)-P [73], HEPO4 (La0.2Ce0.2Nd0.2Sm0.2Eu0.2)
PO4 [73], HEON (Co,Cr,Fe,Mn,Ni)-ON [74] and HEBCN
(Ta0.2Nb0.2Zr0.2Hf0.2W0.2)BCN [75] were reported to have the FCC,
monoclinic, C40-type hexagonal and FCC structures, respectively.
Details regarding the crystal structures of the different types of high-
entropy ceramics are given in Tables A2–A6 of the Appendix.
5. Theoretical/empirical design
High-entropy materials including both alloys and non-metallic ce­
ramics are interesting due to their enhanced properties resulting from
their unique crystal structures. Although various high-entropy materials
have been introduced so far, there are rather limited publications about
the theoretical simulation and computation of the high-entropy mate­
rials due to their complex chemistry [85]. For the prediction of the
structure of a high-entropy material, empirical models based on a
descriptor are also used, although the progress on this issue is still at its
early stages [41]. These theoretical and empirical methods can be used
to understand the stability of high-entropy materials with a given crystal
structure for a desirable property [41]. In this section, the current
progress on both computational methods and descriptors is reviewed
with the focus on the HEOs and HECs, as the two most frequently
investigated types of high-entropy ceramics.
5.1. Theoretical computation
The Gibbs free energy calculations provide quantitative information
regarding the phase stability and phase diagram. The Gibbs free energy
is computed by either first-principles calculations using the density
functional theory (DFT), molecular dynamics simulation or CALPHAD
(Calculation of Phase Diagrams) [41]. The DFT-based methods are
basically good selections to calculate the energy by considering the
chemical complexity of high-entropy materials [228]. However, the
problem of the DFT-based methods is that they are computationally
limited in scale because of the computational time. Therefore,
high-entropy materials with randomly distributed states and many ele­
ments cannot be precisely analyzed by DFT on a small scale. In contrast,
the molecular dynamics simulation can be used at larger lengths within
a shorter computation time, so it is appropriate for covering materials
with many elements. However, the main limit of the molecular dy­
namics simulation is ignoring the interatomic potentials to solve the
complex chemistry of multi-component ceramics [228]. Due to the
recent development of artificial intelligence and machine learning, new
models have attracted attention in recent years [229–232]. In these new
models, artificial intelligence and machine learning are used to analyze
the DFT results for interatomic potentials, and thus the models can fill
the gap between the DFT and molecular dynamics computations. The
use of machine learning potentials leads to the energy calculations at a
time similar to the molecular dynamics simulation with a precision
comparable to the DFT calculations [228]. In this section, some
important studies on the use of computational methods to predict the
stability and properties of high-entropy ceramics are reviewed. Some of
these computations were validated by experimental results, suggesting
the potential of the computational methods for the future design of
high-entropy ceramics [233–239].
5.1.1. Computation of high-entropy oxides
The addition of each element to high-entropy ceramics can signifi­
cantly influence their crystal structure. DFT calculations have been
effectively used to clarify the contribution of individual elements to the
crystal structure of the HEOs. Rak et al. [87] performed the DFT
S. Akrami et al.
Fig. 5. Utilization of classical simulation and random and genetic algorithm
sampling to predict enthalpy, entropy and phase stability in high-entropy ox­
ides. (a) Variations in enthalpy of mixing for different high-entropy oxide sys­
tems with four and five cations, and (b) variations in mixing enthalpy and
entropy versus number of the cations at different temperatures [256].
calculations on (Mg0.1Co0.1Ni0.1Cu0.1Zn0.1)O0.5 with and without the
addition of Li and Sc. They determined the effect of the electronic states
and charge distribution on the structure of these rock-salt oxides. Their
calculations showed that the addition of Sc oxidizes the majority of Cu,
leading to a large shift from the ideal atomic sites, while Co and Ni
cations are less significantly influenced by the Sc addition. The addition
of Li cations oxidizes some amounts of the Co, Ni and Cu and decreases
the lattice constant, which is in good agreement with the experimental
data. In another study, Rak et al. [240] studied the local atomic
configuration and electronic structure of Cu2+ in (MgCoNiZn)1-xCuxO (x
= 0.13, 0.2, 0,.26) by DFT calculations. They concluded that almost 10
% of the CuO6 octahedra is influenced by the Jahn-Teller compression.
Zheng et al. [97] investigated the HEO of Ni, Mg, Cu, Zn and Co for
chemical confinement of lithium polysulfides in Li-S batteries. They
utilized the DFT calculation to study the interfacial binding interactions
between HEO and polysulfide species. Their results indicated that the
simulated bond distance of Li-O in the HEO is less than that reported in
Li2O [241], confirming a strong interaction between the Li and O atoms
in the HEO. However, the binding distance of S-Ni was very close to the
corresponding bond length in the NiS crystal [242]. They concluded that
the synergic contribution of Li-O and S-Ni binding interactions in the
HEO should be responsible for the confinement of the polysulfide [97].
Bhaskar et al. [243] utilized molecular dynamics simulations along
with experiments to indicate the critical influence of the local cationic
stress on the stability of (MgNiCoCuZn)O. Their results showed that the
local stress fields appear due to the Jahn-Teller lattice distortion around
the Cu2+ ions. Lack of minimization of the local stress fields around the
Cu2+ ions results in the formation of a multi-phase material for this
particular composition [243].
There are studies on the application of CALPHAD to predict the
properties of slag melts [244,245]. Although these studies are not
directly related to the HEOs, they suggest that the CALPHAD method can
be used for the simulation of HEOs in the liquid or solid states. Hack
et al. [245] reported the modelling of slag viscosities by the CALPHAD
approach for a fully-liquid SiO2-Al2O3-CaO-MgO-Na2O-K2O-FeO-Fe2O3.
Their results showed a good consistency with the experimental data and
could predict the viscosity of a wide range of compositions [245]. A
similar successful study was performed by Wu et al. [244] for SiO2-A­
l2O3-CaO-MgO-Na2O-K2O-FeO-Fe2O3-P2O5. There are several other
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theoretical/experimental studies about other molten or slag oxide sys­
tems [244–255].
Anand et al. [256] utilized the classical simulation and random and
genetic algorithm sampling strategies to investigate the effect of
configurational entropy on the stability of the rock-salt phase in
multi-component oxides (Mg,Co,Cu,Ni,Zn)O, (Ca,Co,Cu,Ni,Zn)O, (Mg,
Co,Cu,Ni)O, (Mg,Co,Cu,Zn)O, (Mg,Co,Ni,Zn)O and (Mg,Cu,Ni,Zn)O.
They reported that the configurational entropy can decreases the free
energy and stabilize the rock-salt phase in all oxides, but the lowest
temperature for such a stabilization is achieved in (Mg,Co,Cu,Ni)O and
(Mg,Co,Ni,Zn)O with low enthalpies, and the highest temperature is
achieved in (Ca,Co,Cu,Ni,Zn)O with a high enthalpy (Fig. 5a). As illus­
trated in Fig. 5b, they clearly showed that the enthalpy and entropy of
mixing increase by increasing the number of cations, but the increase in
enthalpy compared to the increase in entropy is not very significant for
the systems with three cations or more. The average enthalpy and en­
tropy contribution to the free energy overlaps between four and five
cations, indicating that an average of five cations are required to sta­
bilize the rock-salt phase in this system.
Cassar et al. [257] used the neural network to predict the glass
transition temperature in various multi-component oxide glasses. Their
neural network could predict the published transition temperatures with
a 95 % accuracy, and the related deviations were less than ±6% for 90 %
of the data. Although this study does not deal directly with the HEOs, it
suggests the potential of the neural network to predict the properties of
multi-component systems including HEOs.
5.1.2. Computation of high-entropy carbides
First-principles calculations of HECs by the DFT method has shown
good consistency with the experimental data, suggesting the capability
of the DFT method to predict the phase stability in HECs. Ye et al. [258]
theoretically studied the formation of a single phase in
(Zr0.25Nb0.25Ti0.25V0.25)C by first-principles calculations and reported a
good consistency with the experimental data. In another study, Zhang
et al. [259] investigated the thermodynamics, electronic structure and
mechanical properties of a brittle (TiZrHfNbTa)C by DFT calculations
and reported a good consistency with the experimental data. Their
calculations showed that the length of the metal-carbon bonds in the
solution are slightly different at different sites which leads to a lattice
distortion and a positive effect on the mechanical strength. Zhang et al.
[260] experimentally fabricated B4(HfMo2TaTi)C-SiC and theoretically
examined its atomic structure by DFT calculations. The calculations
successfully predicted the creation of a single-phase HCP structure, in
which the atoms of Hf, Mo, Ta and Ti are distributed on the (0001) plane
and the atoms of C and B are distributed on the (0002) plane.
Jiang et al. [85] investigated the electronic structure and thermo­
dynamic features of two medium-entropy carbides, (HfTaZrTi)C and
(HfTaZrNb)C, by DFT. Both carbides were thermodynamically stable
with negative formation enthalpies. The Debye-Grüneisen model
confirmed that the two carbides illustrate similar trends by increasing
the temperature. These DFT calculations suggested that since (HfTaZrTi)
C has a higher thermal expansion coefficient, it can be more appropriate
for coatings with a thermal stress mismatch, while (HfTaZrNb)C has a
higher strength and is more appropriate for structural applications.
Yang et al. [212] studied the structural, mechanical and electronic
properties of (TaNbHfTiZr)C by DFT calculations at different pressures.
The thermodynamic and elastic stiffness criteria confirmed the stability
of the single-phase (TaNbHfTiZr)C. They found that the HEC has
covalent-ionic features, but the covalent component becomes weaker
than the ionic component under pressure. They also reported that the
HEC shows a brittle-to-ductile transition under 20 GPa. Jiang et al. [261]
also studied the mechanical behavior of (HfTaZrTi)C and (HfTaZrNb)C
under high pressure within the DFT framework. They showed that the
carbon-metal bonding becomes more covalent, the lattice constants
decrease, the unit volume shrinks, the elastic modulus decreases, the
hardness reduces and the Debye temperature decreases with the
S. Akrami et al. Materials Science & Engineering R 146 (2021) 100644

Fig. 6. Utilizing machine learning and DFT methods to calculate the entropy-forming ability (EFA) in the Nb-Hf-Ti-Zr-V-Ta-Mo-W-C high-entropy carbide system. (a)
EFA calculated by machine learning using a random forest fit with 108 chemical attributes versus data from DFT, and (b) EFA calculated by machine learning using a
random forest fit with 108 chemical attributes plus 8 features from CALPHAD versus data from DFT [266].

Fig. 7. Examination of structure of (Hf0.2Zr0.2Ta0.2Nb0.2Ti0.2)B2 by (a–c) DFT calculations and (d) molecular dynamics simulation. Charge density distribution
calculated by DFT for (a) boron (100) layers, (b) metal (100) layers and (c) boron-metal (110) interlayer [269]; (d) general structure of boride constructed by
molecular dynamics simulation [270]. The small pink balls in (d) are boron atoms that are distributed similar to graphene layers and the big balls are Hf, Zr, Ta, Nb
and Ti.

increasing pressure. The Vickers hardness of (HfTaZrNb)C was more
than (HfTaZrTi)C at all pressures, suggesting its potential application
under high pressures.
Zhao [262] examined the lattice distortion of a few HECs with the
rock-salt structure using the DFT calculations. He showed that a signif­
icant distortion occurs in (NbTiVZr)C and (MoNbTaVW)C, leading to the
reduction in the enthalpy of formation and stability of the HECs. He also
found that the lattice distortion leads to the formation of soft and ductile
HECs (due to the electronic charge delocalization), while a high con­
centration of carbon vacancies (resulting from high distortion) improves
the strength of the HECs.
Backman et al. [263] examined the preferential oxidation in re­
fractory high-entropy materials including carbides using analytical and
computational thermodynamic methods. Their results showed that there
is a high tendency for oxidation in the refractory HEAs and HECs con­
sisting elements from groups IV, V and VI of the periodic table, but this
oxidation effect in the carbides is still less compared to the alloys. They
performed experimental verification in another study and confirmed
that their thermodynamic predictions are in good agreement with the
experiments [264].
Wei et al. [265] synthesized a single-phase high-entropy ceramic
(Ti0.2Hf0.2Nb0.2Ta0.2W0.2)C from oxide powders and graphite via car­
bothermal reactive spark plasma sintering. They conducted thermody­
namic calculations by HSC Chemistry 6 software to clarify the
mechanism for the gradient microstructure formation in the HEC. Since
CO and CO2 are also formed during carbothermal reduction, their
thermodynamic calculations confirmed that the formation of a gradient
gas pressure inside the sample leads to the formation of a gradient
microstructure. This finding can be practically used to fabricate HECs
with a gradient structure by controlling the graphite particle size and
resultant gas pressure.
Kaufmann et al. [266] utilized a machine learning method to predict
the ability to synthesize 70 different carbides made from TiC, ZrC, HfC,
VC, NbC, TaC, Mo2C, W2C, WC and Cr3C2 and compared their findings
with the results achieved by DFT calculation. For such predictions, they
calculated the entropy-forming ability with and without including fea­
tures from the CALPHAD method. The entropy-forming ability, which
determines the tendency for a single-phase formation by assessing the
energy distribution, is the inverse of the standard deviation (σ ) of the
energy spectrum above the ground state at zero temperature [267].
EFA (N) = σ[spectrum(Hi (N) ) ]T=0 − 1
(5)

10
S. Akrami et al.
Fig. 8. Application of CALPHAD method to design high-entropy alloys and
corresponding high-entropy hydrides with C14 Laves structure for hydrogen
storage applications. (a) phase diagram of TiZrCrMnFeNi calculated by CAL­
PHAD method, and (b) and (c) experimental X-ray diffraction profiles with
majority of C14 Laves phase for TiZrCrMnFeNi and TiZrCrMnFeNiH6, respec­
tively [271].
√̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅
√∑
√ n g (H − H )2
√ best elements to produce HESs with a low local strain energy. They could
i i mix
√
σ {Hi (N) } = √i=1 ∑ (6)
√ n
( gi ) − 1
i=1
In these equations, EFA is the entropy-forming ability, N is the
number of elements, n is the total number of sampled geometrical
configurations, gi is the degeneracies for the components and Hmix is the
enthalpy of mixture achieved by averaging the enthalpies Hi of the
sampled configurations. As shown in Fig. 6, Kaufmann et al. [266] found
an excellent consistency between the machine learning and DFT
methods. Their calculations led to the experimental synthesis of several
HECs with the rock-salt structure, suggesting the high potential of ma­
chine learning for the design of HECs. Dai et al. [228] also utilized the
machine learning for (Zr0.2Hf0.2Ti0.2Nb0.2Ta0.2)C and showed that the
machine learning in connection with the molecular dynamics simula­
tions is not only suitable for predicting the crystal structure, but also for
predicting the lattice constants, elastic constants and thermal
11
Materials Science & Engineering R 146 (2021) 100644
conductivity of the HECs.
5.1.3. Computation of other high-entropy ceramics
Theoretical computations are not limited to HEOs and HECs and
there are studies of other high-entropy ceramics. Kirnbauer et al. [268]
used DFT calculations to compare the Gibbs free energy of HEN (Hf,Ta,
Ti,V,Zr)N with the Gibbs free energy of FCC-(Hf,Zr)N + FCC-(Ta,V)N +
FCC-TiN and FCC-(Hf,Zr)N + FCC-(Ta,Ti,V)N which are possible
decomposition products of this HEN. The energy calculations up to a
temperature of 1302 K showed that the HEN is energetically more stable
than the two mixtures, but nitrogen loss at high temperature can lead to
the decomposition of HEN.
Wang et al. [269] investigated the crystal structure, electronic fea­
tures and mechanical properties of (Hf0.2Zr0.2Ta0.2M0.2Ti0.2)B2 by DFT
calculations. They reported that the HEB is intrinsically brittle and has a
high Debye temperature with good thermal conductivity. The electronic
structure investigation showed the presence of covalent bonds within
boron layers, metallic bonds within the metal layers and combination of
ionic and covalent bonds between the metals and boron interlayer.
Fig. 7a–c shows the charge density distribution within these layers and
interlayers. Dai et al. [270] used the molecular dynamics simulation to
investigate the temperature dependence of the thermal and elastic
properties of (Ti0.2Hf0.2Zr0.2Nb0.2Ta0.2)B2. The simulated structure, as
shown in Fig. 7d, demonstrates an insignificant lattice distortion in good
agreement with the experimental data. The simulations showed that the
lattice constant and anisotropic thermal expansion increase and the
anisotropic phonon thermal conductivity decreases by increasing the
temperature.
Qin et al. [68] synthesized (Ti0.2Zr0.2Nb0.2Mo0.2W0.2)Si2 by spark
plasma sintering and simulated it by the DFT method. Both energy and
X-ray diffraction simulations were consistent with the experimental
measurements showing the formation of an HCP crystal structure with
the random distribution of the five cations.
Edalati et al. [271] used the CALPHAD method to design new HEAs
and HEHs with the C14-type Laves phase structure for hydrogen storage
applications. The designed alloys were produced by arc melting fol­
lowed by high-pressure hydrogen absorption. The CALPHAD method
suggested the formation of a C14 Laves phase in HEA TiZrMnCrFeNi and
experimental data confirmed the formation of HEA and the corre­
sponding HEH TiZrMnCrFeNiH6 with the Laves phase structures. The
Laves phase hydrides had a low thermodynamic stability and could
reversibly absorb and desorb hydrogen at room temperature. These re­
sults, which are shown in Fig. 8, suggest that the CALPHAD method can
be used to design new HEHs for hydrogen storage applications.
Zhang et al. [69] used a data-driven method for designing HESs with
the appropriate elements to decrease the formation enthalpy and in­
crease the possibility of a single-phase formation. They also used a bond
valence model to calculate the cation-sulfur bond length and select the
design two thermoelectric HESs, Cu5SnMgGeZnS9 and Cu3SnMgInZnS7.
The sulfides were successfully synthesized with a single phase and
showed good thermoelectric properties particularly with some excess
Sn.
5.2. Empirical descriptors
Descriptors are tools that can describe the common properties or the
stability of a single-phase solid solution based on some simple charac­
teristics of the system [41]. Since the selection of a descriptor can in­
fluence the accuracy of the prediction, the choice of the appropriate
descriptor is important. Normally, the descriptors are classified on the
gross, molecular and subangstrom scales [272]. Selecting the best
descriptor is based on the physical/chemical knowledge as well as based
on the data-driven statistics [273]. Despite the good progress of de­
scriptors in various fields of materials science, their use for the
high-entropy ceramics is still in the initial stages [41]. Some of the
S. Akrami et al. Materials Science & Engineering R 146 (2021) 100644

an appropriate tool which can be used to examine the formation of

Fig. 9. Significance of size disorder factor as a descriptor to predict thermal
conductivity of high-entropy oxides with the pyrochlore structure. Thermal
conductivity (k) of 22 single-phase pyrochlores versus the size disorder
parameter (δ∗size ) [175].
single-phase perovskite oxides. Jiang et al. [139], who fabricated pe­
rovskites with a high configurational entropy (≥ 1.5R), used the toler­
ance factor as a descriptor for the design of HEOs. They considered 12
HEOs with the formulation of (SrBa)(M)O3, calculated the Goldschmidt
tolerance factor for all compositions and compared them to the experi­
mental data. They showed that the tolerance factor for all single-phase
perovskites was close to unity (0.97 ≤ tG ≤ 1.03). They suggested that
a tolerance factor close to unity is necessary for forming a single-phase
high-entropy perovskite, although it may not be sufficient. Patel et al.
[146] also investigated the phase diagram and insulator-metallic
behavior of the perovskite (La0.2Pr0.2Nd0.2Sm0.2Eu0.2)NiO3 thin film as
a function of the tolerance factor. They concluded that not only the
crystal structure but also the electronic behavior of the perovskites can
be controlled by the tolerance factor.
Spiridigliozzi et al. [274] introduced a simple descriptor to design
HEOs with the fluorite crystal structure. They systematically studied 18
samples of equiatomic five-component rare earth-based oxides and
showed that the dispersion of the cationic radii of elements is an
important descriptor. They reported when the standard deviations of
distribution of cationic radii is greater than 0.095, a single-phase fluorite
is achieved and when the standard deviation is less than 0.095, a
mixture of fluorite and bixbyite or a single-phase bixbyite is formed.
Wright et al. [175] used the size disorder factor (δ∗size ) as a descriptor
to predict the thermal conductivity of HEOs with the pyrochlore
structure.
√̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅
δ∗size = δ2A + δ2B (7)

where δA and δB are the lattice size differences related to the A and B sites
in the pyrochlore structure, respectively. They suggested that the size
disorder factor as a descriptor is more effective than the ideal mixing
entropy to predict the thermal conductivity. As shown in Fig. 9, their
results showed that the thermal conductivity decreases by increasing the
size disorder factor due to the significant effect of severe lattice distor­
tion on the reducing the thermal conductivity.

5.2.2. Descriptors in high-entropy carbides

HECs are the second highly-investigated high-entropy ceramics and
Fig. 10. Entropy-forming ability as a descriptor to determine the formation of there have been some attempts to define descriptors to predict the
single-phase high-entropy carbides. Correlation between lattice distortion (ε) properties of these ceramics. Sarker et al. [267] utilized the
and reciprocal of entropy-forming ability (EFA− 1). Circles and squares indicate entropy-forming ability as a descriptor to address the ability to synthe­
single-phase and multi-phase compounds, respectively [267]. size hard metal carbides. The entropy-forming ability, described as EFA
in Eq. (5), determines the relative tendency of the material to create a
single-phase high-entropy phase by assessing the energy spectrum of
Table 6
configurationally randomized calculations to create a unit cell. A high
Influence of entropy-forming ability (EFA) on formation of single-phase or
EFA or thin spectrum indicates a low energy barrier to have a random
multi-phase high-entropy carbides [275].
configuration, promoting high entropy and disordering into the system.
Composition EFA (eV/atom) Single or Multiple Phases
Likewise, a low EFA in Eq. (5) or wide spectrum indicates a high energy
Ti0.2Zr0.2Hf0.2Nb0.2Ta0.2)C 100 Single Phase barrier for introducing a random configuration, promoting the forma­
(Ti0.2Hf0.2V0.2Nb0.2Ta0.2)C 100 Single Phase tion of ordered phases. They used this method to investigate 56
(Ti0.2V0.2Nb0.2Ta0.2W0.2)C 77 Single Phase
(Ti0.2Zr0.2Hf0.2Ta0.2W0.2)C 50 Single Phase
five-cation compositions, in which the metals were Hf, Nb, Mo, Ta, Ti, V,
(Ti0.2Hf0.2Nb0.2Ta0.2W0.2)C 67 Single Phase W and Zr. They showed that single phases with a lower lattice distortion
(Ti0.2V0.2Nb0.2Ta0.2Mo0.2)C 100 Single Phase are formed for higher values of the entropy-forming ability, as shown in
(Ti0.2Zr0.2Hf0.2Ta0.2Mo0.2)C 63 Single Phase Fig. 10. They also concluded that since disordering improves the me­
(Ti0.2Hf0.2Nb0.2Ta0.2Mo0.2)C 83 Single Phase
chanical properties, the entropy-forming ability can be used to design
(V0.2Nb0.2Ta0.2Mo0.2W0.2)C 125 Single Phase
(Zr0.2Hf0.2Ta0.2Mo0.2W0.2)C 45 Multiple Phases ultrahard single-phase carbides, such as MoNbTaVWC5, HfNbTaTiZrC5
(Ti0.2Zr0.2Hf0.2Mo0.2W0.2)C 38 Multiple Phases and HfTaTiWZrC5, with hardness values of 32− 33 GPa. Harrington et al.
(Zr0.2Hf0.2V0.2Mo0.2W0.2)C 37 Multiple Phases [275] also used the entropy-forming ability to show the tendency of
HECs to form a single phase. As shown in Table 6, they found that when
the value is greater than 45− 50 eV/atom, a single phase is formed; and
applications of descriptors to design new high-entropy ceramics are now
when the value is lower than 45− 50 eV/atom, multiple phases are
reviewed.
formed.
Ning et al. [276] used the VASP (Vienna Ab-Initio Simulation
5.2.1. Descriptors in high-entropy oxides
Package) code for DFT calculation and introduced the lattice size dif­
As mentioned earlier in Eq. (4), the Goldschmidt tolerance factor is
ference (δ) as a descriptor for investigation of the ability to synthesize

12
 S. Akrami et al.
Fig. 11. Schematic illustration of high-pressure torsion as a solid-state reaction
synthesis method [294].
HECs.
√̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅
√ i=0 (
√∑ ri )2
δ=√ xi 1 −
r based on controlling the interdiffusion in the initial precursor powders
n
where xi , ri and r are the atomic fraction of component i, lattice constant
of component i and the average lattice constant for n components,
respectively. They commented that a smaller lattice size difference, such
as 3.041 %, leads to a smaller lattice distortion and a higher possibility
for the solid-solution formation.
5.2.3. Descriptors in other high-entropy ceramics
In one of the limited attempts to find descriptors for high-entropy
ceramics other than HEOs and HECs, Wen et al. [66] examined the
ability to synthesize an aluminosilicide (Mo0.25Nb0.25Ta0.25V0.25)
(Al0.5Si0.5)2 by thermodynamic calculations and by lattice size differ­
ence evaluation. Both methods suggested the formation of a single phase
in this material with a lattice size difference of 1.893 %.
Liu et al. [277] studied the single-phase formation possibility of HEB
(Ta0.2Nb0.2Ti0.2W0.2Mo0.2)B2 by lattice size difference calculations and
experimental synthesis. They found a lattice size difference of 2.763 %
which is smaller than the value of 3.109 % reported for the single-phase
(Ti0.2Hf0.2Zr0.2Nb0.2Ta0.2)B2 [61], suggesting that the (Ta0.2Nb0.2
Ti0.2W0.2Mo0.2)B2 should have a single phase in good agreement with
their experimental data.
Nygard et al. [223] suggested that the valence electron concentration
can be used as a descriptor to design HEHs with a low thermodynamic
stability. They suggested that a valence electron concentration of 6.4 is
needed to design HEHs with the capability to absorb and desorb
hydrogen at room temperature. Edalati et al. [271] and Floriana et al.
[278] used this descriptor and successfully designed two HEHs for
room-temperature hydrogen storage.
6. Production methods
The synthesis methods play an important role in development of
high-entropy ceramics. The selection of an appropriate synthesis route is
based on several aspects including phase stability, elemental distribu­
tion, product shape, product size, desirable property and application.
There are some other parameters which should also be considered in
selecting a synthesis process, such as time, temperature and complexity
of process. Although bulk samples and thin films are quite important for
mechanical and coating applications, there are some trends to
­
Materials Science & Engineering R 146 (2021) 100644
synthesize high-entropy nanomaterials, including nanoparticles, nano­
rods, nanowires, nanotubes, nanosheets, etc. These nanomaterials can
show better physical and chemical characteristics for some specific ap­
plications compared to their bulk counterparts due to several core effects
such as small size effect, surface effect, quantum size effect, quantum
tunneling effect and dielectric confinement effect [279,280].
The synthesis methods for high-entropy ceramics can be classified
into three main groups: solid-state methods (e.g., ball milling, high-
pressure torsion, sintering, thermal reduction, and self-propagating
high-temperature synthesis), liquid-state methods (e.g., sol-gel, solu­
tion combustion, solvothermal/hydrothermal synthesis, co-
precipitation and hydrothermal treatment, sonochemical-based syn­
thesis, facile electrochemical synthesis, polymeric steric entrapment,
two-step soft urea method, polymeric synthesis, dealloying, nebulized
spray pyrolysis, flame spray pyrolysis and droplet-to-particle aerosol
spray synthesis) and gas-state methods (e.g., sputtering deposition, and
pulsed laser deposition). In this section, the main synthesis routes to
produce high-entropy ceramics are reviewed. It should be noted that
besides these main methods, some other methods have also been used to
synthesize high-entropy ceramics, as summarized in the Appendix.
6.1. Ball milling
Solid-state reaction methods, which are conventional methods to
fabricate high-entropy ceramics [83,91,93,157,158,174,199,200], are
(8)
to produce a high-entropy ceramic product. The most popular solid-state
reaction method is ball milling [118]. In the ball milling method, the
initial powders together with some balls are placed in a vial and sub­
jected to severe rotation or vibration. The collision of the balls with the
vial and powders leads to solid-state reactions. The severity of the
solid-state reaction during ball milling strongly depends on the melting
temperature of the precursors. In the case of low-melting point pre­
cursors, most of the interdiffusion occurs during ball milling even when
processing at room temperature [88]. However, in the case of
high-melting point precursors, ball milling is usually used only for
mixing and the diffusion usually occurs during post-milling heat treat­
ment [118]. It should be noted that the melting point is not the only
determining factor in ball milling and many experimental parameters
including the differences in the hardness of precursors can influence the
synthesis.
Powders of some HECs, such as TiZrHfVNbC5, TiZrHfVTaC5,
TiZrHfNbTaC5, TiZrVNbTaC5, TiHfVNbTaC5 and ZrHfVNbTaC5, can be
directly fabricated by the ball milling of the elemental powders and
without any need for heat treatment [281]. It was also shown that using
the powders of multi-component alloys or intermetallics as the starting
materials can reduce the milling time to produce the HECs [282]. A
combination of ball milling and sintering is quite effective to fabricate
bulk samples. For example, Moskovskikh et al. [283] fabricated two
HECs, Hf0.2Ta0.2Ti0.2Nb0.2Zr0.2C and Hf0.2Ta0.2Ti0.2Nb0.2Mo0.2C, by the
ball-milling of a mixture of metal powders and graphite particles fol­
lowed by spark plasma sintering.
6.2. High-pressure torsion
High-pressure torsion is classified as a severe plastic deformation
method and is mainly used for grain refinement in metallic materials
[284–286]. However, the method has shown high potential for
solid-state synthesis [287–289], reactive cold consolidation of powders
[290–292] and control of phase transformations particularly in ceramics
[293–295]. In this method, as schematically shown in Fig. 11, a bulk disc
or a mixture of compacted powders are placed between two anvils under
a pressure in the range of several giga-Pascals and severely strained by
rotation of the anvils with respect to each other. The method was
recently used to synthesize various high-entropy materials [296]. The
method combined with oxidation, nitriding and hydriding was
13
S. Akrami et al. Materials Science & Engineering R 146 (2021) 100644

improvement of the material structures [311–317]. Reactive spark

plasma sintering includes both sintering and solid-state reactions and is
effectively used to synthesize HECs and HEBs [265,318–321]. Table 7
summarizes some high-entropy ceramics which were sintered or syn­
thesized by this method.

6.3.2. Reactive flash sintering

Flash sintering is used to densify and synthesize (reactive flash sin­
tering) many different ceramics, such as ZnO, TiO2 and ZrO2, at low
temperature and within a short period of time [325–330]. In this
method, electric current and heating are simultaneously applied to a
sample and densification occurs within seconds to minutes [107]. The
facility for flash sintering consists of three main sections: i) furnace for
heating, ii) electric current supply and iii) electrodes which are con­
nected to the sample and power supply [107]. The method combined
with ball milling was used to produce high-entropy ceramics [107,144,
145]. Kumar et al. [106] used the method to synthesize (Mg,Co,Cu,Ni,
Zn)O with a single-phase rock-salt structure at the low temperature of
623 K in 3 min, while the synthesis of this HEO with other thermal
methods requires temperatures higher than 1123 K for several hours. Liu
et al. [107] used the method and synthesized Mg0.2Ni0.2Co0.2Cu0.2Zn0.2O
with single-phase rock-salt structure within a few seconds without any
heating.
Fig. 12. Illustration of spark plasma sintering method which includes elec­
trodes, die, press and vacuum chamber [310].
6.4. Thermal reduction

Table 7 The thermal reduction process is based on the reduction of a reac­

Chemical composition of high-entropy ceramics which were sintered by spark
plasma sintering or synthesized by reactive spark plasma sintering.
Sintered by Spark Plasma Sintering Synthesized by Reactive Spark Plasma
Sintering
(Hf0.2Ta0.2Zr0.2Ti0.2Nb0.2)C-xSiC (Ti0.2Hf0.2Nb0.2Ta0.2W0.2)C [265]
[322]
Hf0.2Ta0.2Ti0.2Nb0.2Zr0.2C [283] (Ti0.2Zr0.2Hf0.2Mo0.2W0.2)B2 [300]
Hf0.2Ta0.2Ti0.2Nb0.2Mo0.2C [283] (Ti0.2Ta0.2Cr0.2Mo0.2W0.2)B2 [300]
(Zr,Ti,Hf,Nb,Ta)C [323] (Zr0.2Hf0.2Nb0.2Ta0.2W0.2)B2 [300]
(Hf0.2Mo0.2Zr0.2Nb0.2Ti0.2)B2 [324] (Zr0.225Hf0.225Ta0.225Mo0.225W0.1)B2 [300]
(Ti0.2Zr0.2Hf0.2Nb0.2Ta0.2)B2 [300]
(Mo0.2Nb0.2Ta0.2Ti0.2W0.2)Si2 [64] (Ti0.2Zr0.2Nb0.2Ta0.2Mo0.2)B2 [300]
(Mo0.2W0.2Cr0.2Ta0.2Nb0.2)Si2 [67]
successfully used to synthesize HEO TiZrHfNbTaO11 for photocatalysis
[297], HEON TiZrHfNbTaO6N3 for photocatalysis [298] and HEH
MgTiVCrFe-H for hydrogen storage [299], respectively.
6.3. Sintering methods
Spark plasma sintering [300] and flash sintering [106,107] are get­
ting popular as synthesis routes to produce bulk high-entropy materials,
although classical types of sintering methods such as hot sintering [95,
139,156,158,195,301,302] and hot press sintering [303,304] are also
used for the synthesis. Recently, some researchers combined flash sin­
tering and spark plasma sintering to accelerate the synthesis densifica­
tion [305–308]. This method, which is called reactive flash spark plasma
sintering, was used to synthesize (Hf0.2Zr0.2Ta0.2Nb0.2Ti0.2)B2 and
(Hf0.2Zr0.2Ta0.2Nb0.2Ti0.2)C [309].
6.3.1. Reactive spark plasma sintering
Spark plasma sintering, which is also known as direct current sin­
tering or field-assisted sintering, is used for the consolidation of nano­
sized powders to high-density bulk samples [300,310]. As shown in
Fig. 12, the sample in this method is placed in a conductive die under
uniaxial pressure and heated by electric pulses from two electrodes
which are located on both sides of the die [310]. Good thermal
efficiency, high sintering activity, short sintering time and low sintering
temperature are some advantages of this method which lead to the
tant, such as metal oxides, by a reduction agent, such as carbon (car­
bothermal reduction), boron (borothermal reduction) and boron carbide
(borocarbothermal reduction). The reactant and reducing agents are
usually mixed by a mechanical method, such as ball milling, then heated
to several hundred degrees Celsius. Some HEBs were fabricated by
borothermal reduction [331,332] and borocarbothermal reduction
[333–338] and some HECs were produced by carbothermal reduction
[313,339,340]. Borothermal reduction is more appropriate to synthesize
HEBs with a low porosity; however, borocarbothermal reduction using
boron carbide as a reducing agent is more appropriate to make porous
HEBs with a low thermal conductivity, because a large volume of CO gas
and B2O3 vapor is released during the borocarbothermal reduction
[341]. The borocarbothermal reduction has some other advantages,
such as low price of starting materials, low processing temperature and
no need for forming and sintering agents. The reactions for borothermal
and borocarbothermal reduction to synthesize
(Zr0.2Hf0.2Ti0.2Nb0.2Ta0.2)B2 are shown in Eqs. (9) and (10), respectively
[341].
6ZrO2 + 6HfO2 + 6TiO2 + 3Nb2O5 + 3Ta2O5 + 104B → 30
(Zr0.2Hf0.2Nb0.2Ta0.2Ti0.2)B2 + 22B2O3(gas) (9)
14ZrO2 +14HfO2 +14TiO2 + 7Nb2O5 + 7Ta2O5 + 52B4C → 70
(Zr0.2Hf0.2Nb0.2Ta0.2Ti0.2)B2 + 34B2O3(gas) + 52CO(gas) (10)
6.5. Self-propagating high-temperature synthesis
Self-propagating high-temperature synthesis, which is based on an
exothermic combustion reaction between reactants, is used to produce
various organic and inorganic materials [342]. The reactants are
sometimes mechanically activated by ball milling [343,344]. However,
in some cases with a high activity, the initial samples are sintered to
decrease the effective surface area and prevent excess exothermic re­
actions [345]. To start the reaction, the reactant mixture is heated in a
small part of the sample and the exothermic reaction automatically
continues. This method is considered more environmentally friendly
compared to traditional solid-solution reaction techniques [346]. This
method combined with spark plasma sintering was successfully used by

14
S. Akrami et al.
Fig. 13. Synthesis of mesoporous high-entropy oxides using mechanochemical nonhydrolytic sol-gel method [349].
Fig. 14. Schematic illustration of (Co0.2Cu0.2Mg0.2Ni0.2Zn0.2)O nanocrystalline powder production by solution combustion synthesis [110].
Tallarita et al. [347] to produce an HEB (Hf0.2Mo0.2Ta0.2Nb0.2Ti0.2)B2
from pure metal and boron powder, based on the exothermic reaction
shown below.
Hf + Mo + Ta + Nb + Ti + 2B → (Zr0.2Mo0.2Ta0.2Nb0.2Ti0.2)B2
6.6. Sol-gel method
The sol-gel synthesis method is among the liquid-state or wet
chemical synthesis methods. This method is a cheap route which can be
used to produce high-purity and high-quality nanoparticles at low
temperatures. The sol-gel process, which can be conducted in the pres­
ence of water (hydrolytic sol-gel) or under dry conditions (non­
hydrolytic sol gel), is based on a reaction between the alkoxide M-OR
(M: metal, O: oxygen, R: alkyl group) and the salt of metals (nitrates M-
NO3 or chlorides M-Cl) to produce an oxide (M-O-M) [348].
M – Cl + M – OR → M – O – M + RCl
The alkoxide can be directly used for the oxide production or it may
be produced by an in-situ reaction between the salt of metals and ether
(R-O-R) or alcohol (ROH) [348].
M – Cl + R – O – R → M – OR + RCl
M – Cl + ROH → M – OR + HCl
This method was used to produce various high-entropy ceramics,
such as (Yb0.2Y0.2Lu0.2Sc0.2Gd0.2)2Si2O7 [197], 4.5SiO2-3Al2O3-1.5­
P2O5-4CaO-1CaF2 [203] and 43SiO2-24.5CaO-24.5Na2O-6P2O5-2Fe2O3
[202].
The mechanochemical nonhydrolytic sol-gel is a combination of the
sol-gel and ball milling methods. Zhang et al. [349] used the method to
Materials Science & Engineering R 146 (2021) 100644
produce (CuNiFeCoMg)x-Al2O3 with the cubic phase and mesoporous
structure for the catalytic oxidation of CO. They mixed the chloride of
metals with aluminum isopropoxide and polyethylene glycol, ball milled
the mixture for 1 h, washed it and calcined it at 673 K (Fig. 13).
(11)
6.7. Solution combustion synthesis
In this method, oxides are synthesized by combustion of a fuel, an
oxidizer and oxygen. Metal nitrates (M-NO3) are usually used as the
oxidizer and glycine (C2H5NO2) as the fuel. The mechanism of this
method is shown by the following formula [110].
M1NO3 + M2NO3 + M3NO3 + M4NO3 + M5NO3 + O2 + C2H5NO2 → HEO
+ H2O + CO2 + N2 (15)
As shown in Fig. 14, metal nitrates, fuel and water are first mixed to
prepare a sol. Hydrated nitrates are preferred to other salts because of
the excellent oxidizing power of NO−3 , their low decomposition tem­
(12) perature and their fine solubility in water [350]. The mixture is then
dried to produce a gel and combustion of the dried mixture is conducted
under elevated temperatures in an electric furnace to produce the HEOs.
The combustion temperature is estimated by the following equation
[350].
/
(13) Tc = T0 + (ΔH 0r + ΔH 0P ) CP (16)
(14)
where T0 , ΔH0r , ΔH0P and CP are room temperature, formation enthalpy of
reactants, formation enthalpy of products and the heat capacity of the
products at a constant pressure, respectively.
This method has some advantages for future commercialization: (i)
time and energy efficiency, ii) easiness and low cost of equipment [351],
iii) applicable to various types of ceramics including oxides, carbides,
borides, etc. [352], iv) synthesis of high-purity complex oxides [350],
15
S. Akrami et al.
Fig. 15. Schematic illustration of sonochemical-based synthesis to produce
nanoparticles of BaSr(ZrHfTi)O3 perovskites [80].
Fig. 16. Schematic of experimental set-up for facile electrochemical synthesis
to produce high-entropy carbides [368].
Fig. 17. Two-step soft urea method for synthesis of high-entropy nitrides from
halide salts of individual elements [372].
and v) production of metastable phases in a short time by controlling the
combustion temperature [353]. Regarding the last merit, Mao et al.
[110] showed that the combustion temperature can be used as an
effective parameter to control the phases in (Co0.2Cu0.2Mg0.2Ni0.2Zn0.2)
O. They showed that the stability of the spinel, wurtzite and tenorite
phases becomes weak by increasing the synthesis temperature to 1073,
1098 and 1123 K and a single-phase rock-salt structure appears by
combustion at temperatures higher than 1123 K. It was also shown that
the fuel type (glycine, urea, citric acid and hexamine) and
fuel-to-oxidizer ratio can be considered as effective parameters to con­
trol crystal structure and crystallinity [354].
Auto-combustion sol gel, which is also known as the citrate gel auto-
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Materials Science & Engineering R 146 (2021) 100644
combustion method [355], is a method combining the solution com­
bustion synthesis and the sol-gel method. In this method, the nitrates of
metals are mixed with citric acid as a complexing agent and fuel [162,
163].
6.8. Solvothermal and hydrothermal synthesis
Thermal synthesis including solvothermal and hydrothermal [356]
methods are based on the crystallization process of substances. The
difference between these two methods is that the reactant is dissolved in
water in the hydrothermal method and in an organic solvent in the
solvothermal method. These two methods are usually conducted in a
sealed autoclave reactor under high temperature and pressure. The
morphology and particle size of the product from these methods can be
controlled by some parameters such as temperature, pH, reactant con­
centrations and surfactant addition [357]. These methods are originally
used to fabricate nanostructured titanium dioxide, graphene, carbon
spheres and chalcogenides in the laboratory. In the case of high-entropy
ceramics, the application of this method in comparison to other thermal
methods does not confront problems such as complicated reaction
equipment, complicated preparation processes, high reaction tempera­
ture and large particle size [103,164]. Wang et al. [82] utilized the
solvothermal synthesis route to produce (CoCuFeMnNi)3O4 with parti­
cle sizes as small as 5 nm.
6.9. Co-precipitation and hydrothermal treatment
This method is usually used to synthesize the oxide-, fluoride- or
oxyfluoride-based nanophosphors [358]. The mechanism of the process
is based on a reaction between the precursors, such as chlorides, nitrates
or acetates, and an alkali such as sodium hydroxide. The precursors are
usually dissolved in a solvent such as distilled water, ethanol, cyclo­
hexane or N,N-dimethyl formaldehyde [358]. The co-precipitation
method can be combined with a hydrothermal treatment to enhance
the material homogeneity. Some HEOs were synthesized by this method
such as (Mg,Co,Ni,Cu,Zn)O [109], Ce0.2Zr0.2Y0.2Gd0.2La0.2O2− σ [120],
(Zn,Mg,Ni,Fe,Cd)Fe2O4 [205] and (La0.2Ce0.2Nd0.2Sm0.2Eu0.2)2Zr2O7
[176].
6.10. Sonochemical-based synthesis
Sonochemical-based synthesis is a precipitation method with an
additional sonication step to accelerate mixing the initial precursors
with alkali (NaOH) using ultrasonic vibrations [80]. Fig. 15 shows a
schematic illustration of the method which was successfully use to
produce BaSr(ZrHfTi)O3, BaSrBi(ZrHfTiFe)O3 and Ru/BaSrBi(ZrHfTiFe)
O3 perovskites with large surface areas [80]. Cavitation phenomenon
caused by high-intensity ultrasound produces a very large energy which
results in easy activation of the reactant molecules and production of
HEOs at room temperature [80].
6.11. Facile electrochemical synthesis
The facile electrochemical synthesis method is mainly used to pro­
duce metals from their oxides [359–362], although the application of
the method has been extended to produce carbides in the last decade
[363–367]. The method was recently utilized to fabricate the (TiNb­
TaZrHf)C ceramics [368]. The setup of method to produce HEC is shown
in Fig. 16 which consists of a cathode (compact mixture of metal oxides
and graphite sintered at 523 K in air for 3 h), an anode (graphite) and an
electrolyte (molten CaCl2 at 1173 K). When a constant voltage is
applied, oxygen ions transfer from the cathode to the anode through the
electrolyte which results in reactions in the cathode and formation of a
carbide, as shown in Fig. 16 [368].
S. Akrami et al.
Fig. 18. Experimental setup for nebulized spray pyrolysis to produce particles of high-entropy oxides [376].
Fig. 19. Schematic illustration of droplet-to-particle aerosol spray synthesis equipped with a carbonized wood micro-channel heater to produce high-entropy oxides
from nitrate salts of individual elements [381].
6.12. Polymeric steric entrapment method
Polymeric steric entrapment is an appropriate route to produce the
homogeneous solid solutions [369,370]. The mechanism of this method
is based on entrapping cations in polyvinyl alcohol structure. In this
method, the initial materials in the form of nitrates are dissolved in
water and polyvinyl alcohol and stirred for a period of time and sub­
sequently heated. After heating, the cations entrapped in the polyvinyl
alcohol structure create a metal oxide with the inorganic part of the
polymer. A calcination treatment is used to decompose the nitrate and
organic polymer and form the pure HEO [195]. This technique was used
by Tseng et al. [195] to synthesize Gd0.4Tb0.4Dy0.4Ho0.4Er0.4O3.
6.13. Two-step Soft urea method
The soft urea strategy is a simple, nontoxic and flexible mechano­
chemical method to produce nitride compounds for different applica­
tions. As shown in Fig. 17, in this method, soft urea and the chlorides of
elements are mixed and ball milled together for a specific time. A metal-
urea gel-like product is then formed which is pyrolyzed under a N2 at­
mosphere [371]. The method was used to successfully fabricate the HEN
of VCrNbMoZr [372].
6.14. Polymeric synthesis
This method is based on the fabrication of a polymer structure. In this
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Materials Science & Engineering R 146 (2021) 100644
method, the nitrate of metals is mixed with water, citric acid and
ethylene glycol to produce a chelate of metals. The reaction mixture is
then heated to remove the water and organic compounds and produce
ceramic compounds [108]. Yoon et al. [108] combined this method with
reactive flash sintering and produced Mg0.2Ni0.2Co0.2Cu0.2Zn0.2O.
6.15. Dealloying method
The dealloying concept originally comes from the corrosion field, but
it is now used as a facile technique to produce nanoporous materials
with large surface areas for different applications such as catalysts,
sensors, actuators, electrolytes, capacitors, high-temperature scaffolds
and anodes of batteries [373]. In the case of high-entropy ceramics,
dealloying in a corrosive sodium hydroxide solution was used to fabri­
cate the HEO of AlFeCoNiCr for application as a bifunctional oxygen
electrocatalyst [374].
6.16. Liquid polymer precursor synthesis
For the liquid polymer precursor method, the precursors in the
polymeric form are subjected to pyrolysis to form high-entropy ce­
ramics. In a successful attempt to use the method for the synthesis of
rare-earth-based HECs, the rare-earth acetylacetonates and metal ace­
tylacetonate alkoxides were mixed together and the mixture underwent
controlled co-hydrolysis and a subsequent polycondensation reaction to
obtain a viscous solution. A carbon source was then added to the mixture
 S. Akrami et al.
Fig. 20. Schematic illustration of sputtering deposition method to synthesize
thin films of the high-entropy nitrides [382].
and pyrolysis was performed to achieve the HEC powders [375].
6.17. Nebulized spray pyrolysis
Nebulized spray pyrolysis is a chemical method for depositing thin
film oxides. In this method, the salts of elements (usually nitrates) are
nebulized (converted to spray) in a chamber using an ultrasonic
generator, then subjected to pyrolysis. As shown in Fig. 18, to produce
HEOs using this method, the salt solutions are mixed with oxygen and
flow into the hot-wall reactor where pyrolysis occurs at high tempera­
ture. After pyrolysis, the HEOs are collected by a filter-based collector,
compacted as a thin film and sintered by thermal treatment [376]. The
reaction rate and oxygen concentration can be adjusted by controlling
the oxygen pressure and temperature using relevant control valves. This
method was used to produce the HEOs (Co0.2Cu0.2Mg0.2Ni0.2Zn0.2)O
[101], (Co0.2Cu0.2Mg0.2Ni0.2Zn0.2)O [102], (Ce0.2La0.2Pr0.2Sm0.2Y0.2)
O2-δ [102], (Gd0.2La0.2Nd0.2Sm0.2Y0.2)(Co0.2 Cr0.2 Mn0.2 Fe0.2 Ni0.2)O3
[102] and (Co,Cu,Mg,Ni,Zn)O [103].
6.18. Flame spray pyrolysis
Flame spray pyrolysis is a synthesis method to produce nanopowders
of various oxides including simple and complex oxides [377]. The
method was used to produce HEOs such as (Co0.2Cu0.2Mg0.2Ni0.2Zn0.2)O
[104] and (Co,Cu,Mg,Ni,Zn)O [103]. In this method, liquid metals with
an oxidizing gas are sprayed into a flame zone where the metal oxide is
produced by combustion [377–380]. The facility for this method con­
sists of i) reactant delivery section, ii) flame and reaction chamber, iii)
collection system and iv) vacuum unit [380]. Compared with other
liquid phase synthesis methods, this method has a short reaction time
and produces a more homogeneous product [380]. Furthermore, the
particle size in this method can be rather easily controlled by changing
the processing conditions [377].
6.19. Droplet-to-particle aerosol spray synthesis
The aerosol spray combined with pyrolysis is used to fabricate
nanostructured ceramics in large amounts from their salts. Wang et al.
[381] downscaled this method to the form of droplet-to-particle aerosol
spray coupled with a carbonized wood microchannel reactor and used it
at 2000 K to produce HEOs such as AuCoCuIrPtMnMoNiPdRuOx and
ZnCoMnNiCuOx. In their study, as shown in Fig. 19, the nitrate of metals
is dissolved in ethanol, converted to droplets and sprayed to the
micro-channel heater by a gas carrier to pyrolyze and manufacture the
HEOs.
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Materials Science & Engineering R 146 (2021) 100644
6.20. Sputtering deposition
Sputtering deposition is a conventional method to produce thin film
materials. This method consists of a substrate, such as a silicon wafer,
and a target, that is an alloy of the desired elements, which are located in
a vacuum chamber. A sputtering gas, such as Ar, is used for the
bombardment of the target and removing the elements. As shown in
Fig. 20, to make the nitride, oxides or carbides, N2, O2 or CH4 are
injected into the vacuum chamber to react with elements and create
deposits on the substrate surface [382]. There are different techniques
for sputtering, such as ion beam sputtering, reactive sputtering, diode
sputtering, radio-frequency sputtering and magnetron sputtering which
were used to produce HENs, HEOs, HEBs, HEONs and HECs such as
Al-Cr-Nb-Y-Zr-N [383], (VAlTiCrMo)Nx [384], (AlCrTaTiZrMo)N [385],
(AlCrTaTiZr)Ox [201], AlxCoCrCuFeNi-O [57], (MgZnMnCoNi)Ox
[386], (CrFeMnCoNi)Ox [386], Zr0.23Ti0.20Hf0.19V0.14Ta0.24B2 [387],
CoCrFeMnNi-ON [74] and TiZrNbTaHf-C [388].
6.21. Pulsed laser deposition
Pulsed laser deposition is a simple method to produce thin films.
Nowadays, this method is used to synthesize simple and complex oxides
with ferroelectric, ferromagnetic and dielectric properties. For this
method, a high-power laser is used to ablate the material from a target
surface. This ablation (melting, evaporation and ionization) creates a
plasma plume after which the evaporated material is collected and
condensed on a substrate [373]. This process can be performed in a
vacuum condition or in the presence of oxygen to create oxide films. This
method was used by Meisenheimer et al. [389] and Kotsonis et al. [112]
to produce (Mg0.25(1-x)CoxNi0.25(1-x)Cu0.25(1-x)Zn0.25(1-x))O and MgxNix
CoxCuxZnxScxO, respectively. In both studies, a mixture of pressed and
sintered oxides was used as the target and ablation was performed using
a 248-nm KrF laser beam.
7. Properties and potential applications
Ceramics, which mainly contain ionic or covalent bonds, have
various applications as structural and functional materials. They have a
higher hardness, higher melting temperature and high oxidation and
corrosion resistance than metallic materials which result in their
application as coating or high-temperature materials. Unlike metallic
materials, which are usually conductors, ceramics can have different
electronic features as conductors, semi-conductors or insulators, leading
to their application in the electrical and electronic industries. Compared
to conventional ceramics, high-entropy ceramics usually exhibit a better
stability with interesting properties due to the cocktail effect, valence
electron distribution, lattice distortion and sluggish diffusion [1–11,15,
16,20,36,45–47,390–399]. In this section, the properties of
high-entropy ceramics including HEOs, HENs, HECs, HEBs, HEHs, etc.,
are reviewed and their potential applications are discussed.
7.1. Properties of high-entropy oxides
HEOs are the most investigated high-entropy ceramics in recent
years [58,400–438]. They have been studied for various properties and
applications including thermomechanical properties, catalytic proper­
ties, ionic conductivity for batteries, magnetic properties, electrical
properties and optical properties. These properties for different kinds of
HEOs are discussed in this section and the most important findings are
explained in detail.
7.1.1. Thermomechanical properties
Thermal conductivity is defined as the ability of a material to
conduct heat which is determined by the transportation of phonons and
electrons [41]. Ceramics with a low thermal conductivity can be used for
thermal insulation or for thermal barrier coatings to protect the metallic
S. Akrami et al. Materials Science & Engineering R 146 (2021) 100644

Table 8
Reported thermal and mechanical properties of high-entropy oxides.
High-Entropy Oxide Thermal Thermal Elastic Hardness Strength Thermal Expansion
Conductivity Stability (K) Modulus (GPa) (MPa) Coefficient (x10− 6
(Wm− 1 K− 1) (GPa) K-1)

MgxNixCuxCoxZnxO, x = 0.2 [441] 2.95 ± 0.25 152.0 ± 10.6

MgxNixCuxCoxZnxScxO, x = 0.167 [441] 1.68 ± 0.13 236.7 ± 15.9
MgxNixCuxCoxZnxSbxO, x = 0.167 [441] 1.41 ± 0.17 158.4 ± 10.9
MgxNixCuxCoxZnxSnxO, x = 0.167 [441] 1.44 ± 0.10 180.8 ± 17.9
MgxNixCuxCoxZnxCrxO, x = 0.167 [441] 1.64 ± 0.24 151.0 ± 9.2
MgxNixCuxCoxZnxGexO, x = 0.167 [441] 1.60 ± 0.14 229.9 ± 21.2
(Ce0.2Zr0.2Hf0.2Sn0.2Ti0.2)O2 [448] 1.28
La2(Hf1/2Zr1/2)2O7 [175] 2.29 ± 0.06 250.2 ± 4.2
Sm2(Sn1/4Ti1/4Hf1/4Zr1/4)2O7 [175] 1.73 ± 0.05 250.2 ± 4.7
Gd2(Sn1/4Ti1/4Hf1/4Zr1/4)2O7 [175] 1.58 ± 0.05 229.4 ± 4.4
(Sm1/2Gd1/2)2(Ti1/3Hf1/3Zr1/3)2O7 [175] 1.47 ± 0.04 242.0 ± 4.2
(Eu1/2Gd1/2)2(Ti1/3Hf1/3Zr1/3)2O7 [175] 1.52 ± 0.05 243.1 ± 4.0
(La1/2Pr1/2)2(Sn1/3Hf1/3Zr1/3)2O7 [175] 2.24 ± 0.07 275.5 ± 7.9
(Eu1/2Gd1/2)2(Sn1/3Hf1/3Zr1/3)2O7 [175] 2.24 ± 0.07 253.3 ± 4.3
(La1/3Pr1/3Nd1/3)2(Hf1/2Zr1/2)2O7 [175] 2.16 ± 0.06 240.0 ± 4.3
(Sm1/3Eu1/3Gd1/3)2(Hf1/2Zr1/2)2O7 [175] 1.97 ± 0.06 235.7 ± 3.8
(Sm1/3Eu1/3Gd1/3)2(Sn1/3Hf1/3Zr1/3)2O7 [175] 2.21 ± 0.07 256.7 ± 4.1
(Sm1/3Eu1/3Gd1/3)2(Ti1/4Sn1/4Hf1/4Zr1/4)2O7 [175] 1.67 ± 0.05 260.4 ± 5.0
(Sm1/4Eu1/4Gd1/4Yb1/4)2(Ti1/4Sn1/4Hf1/4Zr1/4)2O7 [175] 1.45 ± 0.04 249.4 ± 4.0
(Sm1/3Eu1/3Gd1/3)2(Ti1/2Sn1/6Hf1/6Zr1/6)2O7 [175] 1.71 ± 0.05 280.1 ± 6.2
(Sm1/3Eu1/3Gd1/3)2(Ti3/4Sn1/12Hf1/12Zr1/12)2O7 [175] 1.90 ± 0.06 273.6 ± 5.3
(Sm1/3Eu1/3Gd1/3)2Ti2O7 [175] 2.88 ± 0.09 281.3 ± 5.0
(Sm1/4Eu1/4Gd1/4Yb1/4)2(Ti1/2Hf1/4Zr1/4)2O7 [175] 1.36 ± 0.04 238.3 ± 2.5
(Sm3/4Yb1/4)2(Ti1/2Zr1/2)2O7 [175] 1.40 ± 0.04 227.7 ± 2.5
(La1/5Ce1/5Nd1/5Sm1/5Eu1/5)2Zr2O7 [175] 2.06 ± 0.06 230.6 ± 2.9
(La1/7Ce1/7Pr1/7Nd1/7Sm1/7Eu1/7Gd1/7)2(Hf1/2Zr1/2)2O7 [175] 1.97 ± 0.06 242.0 ± 3.5
(La1/7Ce1/7Pr1/7Nd1/7Sm1/7Eu 1/7Gd1/7)2(Sn1/3Hf1/3Zr1/3)2O7 [175] 2.02 ± 0.06 187.0 ± 5.0
(La0.2Nd0.2Sm0.2Eu0.2Gd0.2)2Zr2O7 [83] <1 1573
(Y0.2Nd0.2Sm0.2Eu0.2Gd0.2)2Zr2O7 [83] <1 1573
(La0.2Y0.2Sm0.2Eu0.2Gd0.2)2Zr2O7 [83] <1 1573
(La0.2Nd0.2Y0.2Eu0.2Gd0.2)2Zr2O7 [83] <1 1573
(La0.2Nd0.2Sm0.2Y0.2Gd0.2)2Zr2O7 [83] <1 1573
(La0.2Nd0.2Sm0.2Eu0.2Y0.2)2Zr2O7 [83] <1 1573
(Hf0.25Zr0.25Ce0.25Y0.25)O2-δ [118] 1.74 ± 0.15 13.6 ± 0.5
(Hf0.25Zr0.25Ce0.25)(Y0.125Yb0.125)O2-δ [118] 1.55 ± 0.20 12.7 ± 0.7
(Hf0.2Zr0.2Ce0.2)(Y0.2Yb0.2)O2-δ [118] 1.29 ± 0.11 13.3 ± 0.6
(Hf0.25Zr0.25Ce0.25)(Y0.125Ca0.125)O2-δ [118] 1.10 ± 0.20 13.3 ± 0.6
(Hf0.25Zr0.25Ce0.25) (Y0.125Gd0.125)O2-δ [118] 1.17 ± 0.13 13.2 ± 0.5
(Hf0.2Zr0.2Ce0.2)(Y0.2Gd0.2)O2-δ [118] 1.61 ± 0.13 13.1 ± 0.5
(Hf0.2Zr0.2Ce0.2)(Yb0.2Gd0.2)O2-δ [118] 1.62 ± 0.13 12.6 ± 0.5
(Hf0.25Zr0.25Ce0.25)(Yb0.125Gd0.125)O2-δ [118] 1.81 ± 0.14 12.3 ± 0.7
(Hf0.314Zr0.314Ce0.314Y0.029Yb0.029)O2-δ [39] 1.78 ± 0.05 201.2 ± 2.2 17.1 ± 1.8
(Hf0.284Zr0.284Ce0.284Y0.074Yb0.074)O2-δ [39] 1.74 ± 0.05 232.8 ± 2.2 17.7 ± 1.7
(Hf0.2Zr0.2Ce0.2Y0.2Yb0.2)O2-δ [39] 2.23 ± 0.07 232.6 ± 2.4
(Hf0.314Zr0.314Ce0.314Y0.029Ca0.029)O2-δ [39] 1.65 ± 0.05 180.1 ± 4.8 18.4 ± 1.3
(Hf0.284Zr0.284Ce0.284Y0.074Ca0.074)O2-δ [39] 1.54 ± 0.05 153.8 ± 2.3 19.6 ± 0.6
(Hf0.314Zr0.314Ce0.314Y0.029Gd0.029)O2-δ [39] 1.74 ± 0.05 199.4 ± 2.0 18.5 ± 1.4
(Hf0.284Zr0.284Ce0.284Y0.074Gd0.074)O2-δ [39] 1.70 ± 0.05 218.9 ± 2.3 18.2 ± 1.7
(Hf0.2Zr0.2Ce0.2Y0.2Gd0.2)O2-δ [39] 2.19 ± 0.06 238.9 ± 2.7 16.3 ± 1.2
a) 11.4 ± 0.5
(Hf0.314Zr0.314Ce0.314Y0.029Yb0.029) O2-δ [446] b) 9.5
c) 2.6
a) 12.2 ± 0.5
(Hf0.284Zr0.284Ce0.284Y0.074 Yb0.074)O2-δ [446] b) 8
c) 4.5
a) 11.6 ± 0.4
(Hf0.2Zr0.2Ce0.2Y0.2Yb0.2)O2-δ [446] b) 9.1
c) 2.9
(Dy0.2Ho0.2Er0.2Y0.2Yb0.2)3NbO7 [456] 0.724 9.51 10.2
(Co,Cr,Fe,Mn,Ni)3O4 [157] 9.70 ± 0.16
(Co,Cr,Fe,Mg,Mn)3O4 [157] 9.76 ± 0.18
(Cr,Fe,Mg,Mn,Ni)3O4 [157] 8.81 ± 0.26
(Al0.19Cr0.13Nb0.19Ta0.30Ti0.19)O2 [196] 1473 410 24
a) 2.57 ± 0.07
(Yb0.25Y0.25Lu0.25Er0.25)2SiO5 [199] b) 8.07 ± 0.13
c) 9.98 ± 0.10
(Co,Cr,Fe,Mn,Ni)3O4 [158] 1273 K
(AlCrTaTiZr)Ox [201] 260 20
(Y1/4Ho1/4Er1/4Yb1/4)2SiO5 [198]
AlxCoCrCuFeNi-O [57] 773 25.7 ± 2.3
(La0.2Ce0.2Nd0.2Sm0.2Eu0.2)2Zr2O7 [176] 0.76
(La0.2Ce0.2Nd0.2Sm0.2Eu0.2)2Zr2O7 [177] 0.86 1873 257 12.42 11
(continued on next page)

19
 S. Akrami et al. Materials Science & Engineering R 146 (2021) 100644

Table 8 (continued )
High-Entropy Oxide Thermal Thermal Elastic Hardness Strength Thermal Expansion
Conductivity Stability (K) Modulus (GPa) (MPa) Coefficient (x10− 6
(Wm− 1 K− 1) (GPa) K-1)

AlxCoCrCuFeNi-O (x = 0.5, 1, 2) [56] 22.6 ± 1.6

0.066Na3PO4+0.034Na2B4O7+0.006Na2WO4+0.1Ni 1073
(CH3COO)2+0.025 Cu(CH3COO)2 coating on Ti [248]
Al0.3CoCrFeMnNi+3 vol.% Y2O3 [209] 1759
(Y0.25Yb0.25Er0.25Lu0.25)2(Zr0.5Hf0.5)2O7 [78] 1.4 8.97
CrFeCoNiMn-O [443] 270 27
10La2O3-20TiO2-10Nb2O5-20WO3-20ZrO2 [206] 6.8
(Al0.31Cr0.20Fe0.14Ni0.35)O [444] 205 18.5
MgxNixCoxCuxZnxScxO (x~0.167) [112] 1273
a) 12.04
(Y0.2Nd0.2Sm0.2Eu0.2Er0.2)AlO3 [147] 4.1 b) 7.46
c) 11.28
(Mg,Co,Ni,Cu,Zn)O [100] 108 ± 5 323 ± 19
(Hf0.314Zr0.314Ce0.314Y0.029Yb0.029) O2-δ [446] 11.4 ± 0.5
(Hf0.284Zr0.284Ce0.284Y0.074 Yb0.074)O2-δ [446] 12.2 ± 0.5
(Hf0.2Zr0.2Ce0.2Y0.2Yb0.2)O2-δ [446] 11.6 ± 0.4

surfaces of high-temperature systems such as turbines or jet engines
[187,439]. Besides a low thermal conductivity, high thermal stability
and appropriate thermal expansion matching with the substrate are
other features of thermal barrier coating ceramics [131,440]. These
properties can be achieved in high-entropy ceramics by manipulating
different kinds of cations and anions in the lattice [441]. HEOs are
known for their low thermal conductivity which is caused by phonon
scattering by multi-components and distorted lattices [118]. Since the
elastic modulus to thermal conductivity ratio indicates the rate of
phonon scattering [441,442], the thermal properties of HEOs are usually
investigated along with their mechanical properties [56,57,78,100,147,
Fig. 21. Low thermal conductivity and high ratio of elastic modulus to thermal
conductivity for high-entropy oxides compared to other materials at room
temperature. (a) Thermal conductivity (k) plotted versus elastic modulus (E)
and (b) E/k ratio for entropy-stabilized oxides (ESOs) compared to other ma­
terials. J14: MgxNixCuxCoxZnxO (x = 0.2), J30: MgxNixCuxCoxZnxScxO (x =
0.167), J31: MgxNixCuxCoxZnxSbxO (x = 0.167), J34: MgxNixCuxCoxZnxSnxO (x
= 0.167), J35: MgxNixCuxCoxZnxCrxO (x = 0.167) and J36: MgxNixCux
CoxZnxGexO (x = 0.167) [441].
157,158,176,177,196,198,199,201,206,209,248,443–446]. The ther­
mal and mechanical properties of HEOs are summarized in Table 8 and
some of the major findings are reviewed below.
Braun et al. [441] studied the thermal and mechanical features of
single-phase Mg0.2Ni0.2Cu0.2Co0.2Zn0.2O, Mg0.167Ni0.167Cu0.167
Co0.167Zn0.167Sc0.167O, Mg0.167Ni0.167Cu0.167Co0.167Zn0.167Sb0.167O,
Mg0.167Ni0.167Cu0.167Co0.167Zn0.167Sn0.167O, Mg0.167Ni0.167Cu0.167
Co0.167Zn0.167Cr0.167O and Mg0.167Ni0.167Cu0.167Co0.167Zn0.167Ge0.167O
and illustrated that disordering of the localized ionic charge can
decrease the thermal conductivity without reducing the mechanical
stiffness. A detailed examination confirmed that these single-phase
HEOs show similar thermal conductivities to the corresponding amor­
phous phases in good agreement with the minimum theoretical limits.
As shown in Fig. 21a and b, these materials show one of the highest
elastic modulus to thermal conductivity ratios reported so far for
isotropic crystals. Braun et al. [441] reported that the six-cation systems
show thermal conductivities two times lower than the five-cation sys­
tems. This latter finding agrees well with the results reported by Liu et al.
[447], who reported that the thermal conductivity decreases when the
entropy increases and the minimum amount of thermal conductivity is
achieved only in the presence of five or six cations.
Chen et al. [448] introduced (Ce0.2Zr0.2Hf0.2Sn0.2Ti0.2)O2 as a
thermally-stable fluorite oxide at 1773 K which shows a reversible
transition into multiple phases at low temperatures and into a single
phase at high temperatures. They reported a low thermal conductivity of
1.28 Wm− 1 K− 1 which is half the thermal conductivity of
yttria-stabilized zirconia (a commercial material used for thermal bar­
rier coating).
Li et al. [83] investigated the rare-earth-based zirconate HEOs with
the single-phase pyrochlore structures as thermal barrier coatings. Their
studies showed that the materials have a good stability at 1773 K which
is a typical temperature for thermal barrier coatings [187,449,450].
Moreover, the thermal conductivity of these HEOs in the temperature
range of 573–1473 K was below 1 Wm− 1 K− 1 which is 50 % lower than
that of yttria-stabilized zirconia. They also suggested that the lattice
distortion and high phonon scattering are the main reasons for the low
thermal conductivity of the high-entropy pyrochlores [51].
Gild et al. [118] studied the thermal behavior and mechanical
properties of eight types of fluorites, which usually have a high hard­
ness, low thermal conductivity, high oxygen vacancy concentration and
high melting temperature. They found that (Hf0.25Zr0.25Ce0.25)
(Y0.125Ca0.125)O2-δ shows the lowest thermal conductivity of 1.10 ± 0.20
Wm− 1 K− 1 with the highest hardness of 13.3 ± 0.6 GPa.
Wright et al. [39] investigated nine fluorite oxides in terms of their
thermal conductivity and mechanical properties. In comparison to
yttria-stabilized zirconia, their materials showed low thermal conduc­
tivity by preserving the high elastic modulus of 210 GPa and high

20
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S. Akrami et al.
Fig. 22. Lower thermal conductivity of high-entropy oxides compared to yttria-
stabilized zirconia. Thermal conductivity (k) versus temperature measured for
several high-entropy oxides and yttria-stabilized zirconia and calculated values for
(Hf0.284Zr0.284Ce0.284Y0.074Yb0.074)O2 (4M) and (Hf0.284Zr0.284Ce0.284Y0.074Ca0.074)O2
(5M) by using Cahill model for phonon limits [39].
hardness of 18 GPa. For the materials with an equiatomic fraction of
cations, the thermal conductivity decreased by increasing the temper­
ature due to Umklapp scattering at low temperatures, but increased at
Fig. 23. High-entropy oxides as new photocatalysts with a high light absorbance and good activity for photocatalytic hydrogen production. (a, b) High-resolution
transmission electron microscopy images and corresponding fast Fourier transform diffractograms, (c) UV–vis light absorbance spectra compared to binary oxides,
and (d) photocatalytic hydrogen generation versus time for three cycles [297].
21
Materials Science & Engineering R 146 (2021) 100644
higher temperatures due to radiative effects, as shown in Fig. 22. For the
materials with a non-equiatomic fraction of cations, an amorphous-like
tendency [442] between the thermal conductivity and temperature
appeared at which the thermal conductivity slowly increased by raising
the temperature or remained approximately temperature-independent.
The thermal conductivity of HEOs with an equiatomic fraction of cat­
ions was higher than the thermal conductivity of the non-equiatomic
ones, despite the lower entropy of the equiatomic ones. The high ther­
mal conductivity of the equiatomic systems was attributed to the va­
cancy clustering effect on reducing the phonon scattering [451–455].
Wright et al. [39] also investigated the elastic modules to thermal
conductivity ratio for their materials and found that the ratio increases
by moving from the non-equiatomic to equiatomic fractions (i.e, phonon
scattering increases by increasing the vacancy concentration). Further­
more, they showed that when the concentration of vacancies is higher
than 5 %, vacancy clustering occurs resulting in the thermal conduc­
tivity enhancement and the Young’s modulus to thermal conductivity
ratio reduction [39].
Zhu et al. [456] reported a low thermal conductivity of 0.724 Wm− 1
K− 1 at room temperature for a niobate (Dy0.2Ho0.2Er0.2Y0.2Yb0.2)3NbO7
with the fluorite structure. This thermal conductivity value is lower than
many HEOs and lower than yttria-stabilized zirconia which suggests the
high potential of this material for thermal barrier coating applications.
Wright et al. [446] investigated the thermal expansion and ablation
of single-phase fluorite oxides [Hf(1− 2x)/3Zr(1− 2x)/3Ce(1− 2x)/3YxYbx]O2-δ
(x = 0.2, 0.074, and 0.029) as potential protective coating materials.
S. Akrami et al.
Fig. 24. High-entropy alloys coupled with high-entropy oxides as active
bifunctional electrocatalyst for Zn-air batteries. (a) Schematic illustration of Zn-
air battery, (b) voltage and power density versus current density achieved in
Zn-air batteries using AlFeCoNiCr alloy and its oxide as bifunctional electro­
catalyst in comparison to using Pt/C-IrO2 electroctalysts [374].
They showed that the intrinsic thermal expansion coefficients for these
oxides are greater than that of yttria-stabilized zirconia and they are
more compatible to the Ni-based superalloys. They found the highest
thermal expansion coefficient for (Hf0.284Zr 0.284Ce0.284Y0.074Yb0.074)
O2-δ due to the oxygen clustering effect. They showed that the molten
salt infiltration and interaction at intermediate temperatures
(1473− 1573 K) is less than the yttria-stabilized zirconia, but increases at
higher temperature due to the higher chemical reactivity.
7.1.2. Catalytic properties
High-entropy ceramics have been considered as potential candidates
to fabricate cheap and high performance catalysts. They have been used
not only as catalysts, electrocatalysts or photocatalysts but also as sup­
ports for catalysts in various applications [457]. In this section, some of
the main findings regarding the catalytic properties of HEOs are
reviewed.
7.1.2.1. Electrocatalytic oxygen evolution reaction. The electrocatalytic
oxygen evolution reaction is a reaction that occurs during water splitting
and in metal-air-batteries [458–463]. Currently ruthenium oxide (ReO2)
and iridium oxides (IrO2) are considered for this application, but their
kinetics and electrochemical efficiency are still low [464]. Introducing
active and stable electrocatalysts with a low cost for the oxygen evolu­
tion reaction is essential for the next generation of energy storage sys­
tems [207]. The oxygen evolution reaction occurs in four main steps, as
described below [465].
CAT* + OH− → CATOH* + e−
−
CATOH* + OH → CATO* + H2O + e −
CATO* + OH− → CATOOH* + e−
CATOOH* + OH− → CAT* + H2O + O2 + e−
Materials Science & Engineering R 146 (2021) 100644
where * indicates the active sites for absorbing OH− and CAT refers to the
catalyst.
In one of the earlier attempts to use high-entropy ceramics as an
electrocatalyst, Wang et al. [82] synthesized (Co,Cu,Fe,Mn,Ni)3O4 with
the spinel structure using the low-temperature solvothermal method and
employed it for the oxygen evolution reaction. In this study, hydrophilic
multi-walled carbon nanotubes were added to the HEO for electro­
catalytic performance [82]. They observed that the Co2+, Fe2+, Mn2+
and Ni2+ ions on the surface of the catalyst are partially oxidized to
Co3+, Fe3+, Mn3+ and Ni3+, respectively. They confirmed that both HEO
and HEO mixed with carbon nanotubes show a perfect performance as
an electrocatalyst, although the charge transfer and overall performance
of the HEO mixed with carbon nanotubes are superior. They obtained
the high current density of 10 mAcm− 2 in 1 M KOH at 1.58 V.
In addition to the electrocatalyst itself, the support for electro­
catalysts is of importance for water splitting. Ding et al. [207] synthe­
sized a high-entropy bulk porous nanostructure by dealloying the
FeCoNiCrNb alloy so that the core was a nanosized intermetallic alloy
and the shell was a nanostructured HEO thin film. The designated ma­
terial illustrated a high surface area, quick dynamics, good long-term
persistence and high electrocatalytic activity for the oxygen evolution
reaction.
7.1.2.2. Photocatalytic hydrogen generation. Photocatalytic hydrogen
generation by water splitting is a clean technology to produce hydrogen,
but the activity of the current photocatalysts is still quite low. Significant
researches are being performed all around the world to find new ma­
terials that can act as active photocatalysts. Edalati et al. [297] syn­
thesized a dual-phase TiZrHfNbTaO11 ceramic with the monoclinic
(Fig. 23a) and orthorhombic (Fig. 23b) structures by high-pressure
torsion followed by oxidation at high temperature and used it as a
photocatalyst for water splitting. The material showed a higher light
absorbance compared to all binary oxides in the Ti-Zr-Hf-Nb-Ta-O sys­
tem, as shown in Fig. 23c, and could successfully produce hydrogen by
photocatalytic water splitting, as shown in Fig. 23d [297]. Lei et al.
[204] could also synthesize the TaNbHfZrTi oxide with a high surface
area in the form of nanotube arrays, but they did not examine the cat­
alytic activity of their material. These studies introduced the
high-entropy photocatalysts as potential candidates for water splitting
applications.
7.1.2.3. Catalytic CO oxidation. Due to the toxicity of CO gas, its fast
conversion or oxidation using appropriate catalysts is a requirement. In
an attempt to address this issue, BaSrBi(ZrHfTiFe)O3 and Ru/BaSrBi
(ZrHfTiFe)O3 with single-phase perovskite structures were synthesized
by the sonochemical-based method as catalysts for CO oxidation, and
their performances were compared to the conventional BaRuO3 catalyst
[80]. It was found that Ru/BaSrBi(ZrHfTiFe)O3 shows a better activity
for the CO conversion compared to BaSrBi(ZrHfTiFe)O3 and BaRuO3 and
can convert 100 % CO to CO2 at 383 K. The lower activity of BaSrBi
(ZrHfTiFe)O3 was attributed to the absence of Ru atoms as the active
sites.
In another attempt, Xu et al. [466] fabricated a high-entropy fluorite
oxide (CeZrHfTiLa)Ox by mechanical milling followed by calcination
and utilized it is as a support to stabilize the Pd single-atom catalyst for
CO oxidation. They showed that Pd atoms are stabilized into the HEO by
forming Pd-O-M bonds (M: Ce, Zr, La). They found that this composition
compared to the typical Pd catalyst on a CeO2 support can have a better
low-temperature CO oxidation activity and superior resistance to ther­
(17) mal and hydrothermal degradation.
Chen et al. [467] made a catalyst from (NiMgCuZnCo)O and CuCeOx.
(18)
The CuCeOx–HEO catalysts showed a high catalytic activity for the CO
(19) oxidation at high temperatures as 1173 K.
(20)
7.1.2.4. Bifunctional electrocatalysis in metal-air batteries.
22
S. Akrami et al.
Fig. 25. Application of high-entropy oxides as catalysts and chemical immobilizer of polysulfide in Li-S batteries. (a) Schematic illustration of utilizing
(Co0.2Cu0.2Mg0.2Ni0.2Zn0.2)O in cathode of Li-S battery, and (b) cyclic voltammetry (current versus voltage) curves of Li-S battery achieved under three conditions:
using a mixture of Ketjen Black (KB) carbon and high-entropy oxide (HEMO-1), using only Ketjen Black carbon, and without using any catalyst and Li2S6 [97].
Electrocatalysts play an important role in the performance of
rechargeable metal-air batteries, but the electrocatalysts in these bat­
teries are usually made from precious materials such as Pt and IrO2. In
an attempt to find cheaper electrocatalysts, The AlFeCoNiCr alloy and its
oxide were used as a bifunctional electrocatalyst with aluminide-oxide
coupling in Zn-air batteries [374]. They reported that utilizing this
bifunctional electrocatalyst in an aqueous Zn-air battery results in
delivering a potential of 1.55 V and a high specific capacity of ~800
mAhg− 1, while its utilization in the solid-state Zn-air batteries results in
a small discharge/charge potential gap of 0.76 V with a good stability
during cycling. As shown in Fig. 24, the performance of this battery was
better than the typical Pt/C-IrO2-based batteries. The results showed
that using the five-element high-entropy components is better than the
three-element components for electrocatalysis due to the effect of de­
fects on enhancement of the electron conductivity.
7.1.2.5. Catalysis and immobilizing in lithium-sulfur batteries. Lithium-
sulfur (Li-S) batteries are considered as potential candidates for the next
generation of rechargeable batteries due to advantages such as a high
nominal capacity of 1675 mAhg− 1, high energy storage density of 2500
kW kg− 1, low price, high safety and abundance of sulfur resources [97,
468–472]. However, they have some disadvantages, such as compli­
cated multi-electron conversion and insulating property of sulfur and
insulating property and shuttle effect of lithium polysulfides, which lead
to the decreasing cyclic capacity and lowering the coulombic efficiency
[97,473–477]. To solve these problems, there have been some efforts to
include catalysts in the cathode [478–483]. Mesoporous carbon and
carbon nanotubes are common host materials in cathodes for encapsu­
lating the sulfur and confining polysulfides by physical immobilization
[484–488]. Recently, HEOs have been considered as catalysts to confine
the polysulfides by chemical immobilization [489–492]. The HEOs
exhibit a better performance than binary oxides due to the synergistic
immobilization effect between the different metal ions [493–496]. The
distribution of various cations in the HEOs provides active sites to
confine the polysulfides during the charging and discharging process.
Moreover, these HEOs show a good thermodynamic and chemical sta­
bility and fine uniformity without any agglomeration of elements, even
after a thermal treatment at 1273 K [204].
Zheng et al. [97] successfully utilized (Co0.2Cu0.2Mg0.2Ni0.2Zn0.2)O
together with carbon as a catalyst and immobilizer in the Li-S batteries,
as shown in Fig. 25a. They showed that the active elements in this HEO
accelerate the redox reaction in the cathode. They also showed that the
synergistic contribution of Li–O and S–Ni bonds from the interaction
between the HEO and lithium polysulfides decreases the shuttle of
polysulfides. They showed that the use of HEO as a catalyst produced a
good reversible capacity, superior cyclic stability and the low-capacity
decay of 0.077 % per cycle after 600 cycles. They confirmed that a
combination of HEO and carbon improves the performance of the
23
Materials Science & Engineering R 146 (2021) 100644
battery compared to using only carbon, as shown in Fig. 25b.
7.1.2.6. Catalytic CO2 conversion. The conversion of CO2 to useful
components, such as CO or fuels, is one strategy to reduce the CO2
emission into the atmosphere. This process is usually conducted at high
temperature in the presence of a catalyst and a reducing agent such as
hydrogen. Chen et al. [94] synthesized Pt/Ru(NiMgCuZnCo)O by a
mechanochemical route under ambient conditions and used it as a
catalyst for the CO2 to CO conversion. They achieved 45.4 % and 47.8 %
CO2 conversions at 773 K within 2 h for the HEOs containing 5 wt% of
Ru and Pt, respectively. They attributed the good performance of these
catalysts, which also showed a good stability at high temperature, to the
fine dispersion of noble metal atoms in the (NiMgCuZnCo)O.
7.1.2.7. Catalytic activity for electrochemical capacitors. Electrochemical
capacitors, including electric double-layer capacitors and pseudo-
capacitors, have a higher power or energy density and longer lifetime
compared with batteries and dielectric capacitors for energy storage
[162]. Metal oxides, such as MnO2, TiO2, RuO2, NiO and Fe3O4, are
usually used as electrodes for pseudo-capacitors, but carbon nanotubes
with a high electrical conductivity and high specific surface area are
used as electrodes for electric double-layer capacitors [497]. Lal et al.
[162] used the HEO, Ni-Fe-Co-Cr-Al-O, as a catalyst for the growth of
carbon nanotubes during the chemical vapor deposition technique and
finally used the mixture of HEO and carbon nanotubes as an electrode in
electrochemical capacitors. The mixture, which had a superior specific
surface area of ~151 m2 g− 1 with a uniform distribution of catalysts,
showed a high electrochemical activity and good physicochemical sta­
bility. They used the polyvinyl alcohol/sulfuric acid hydrogel as an
electrolyte and achieved a complete 100 % capacitance retention with
the high specific capacitance of 286.0 Fg− 1 for up to 15,000 cycles.
7.1.2.8. Catalytic combustion. Cerium oxide with a high oxygen storage
capacity is used as a catalyst in catalytic combustion reactions such as
the water-gas shift reaction [498–501], dry reforming reaction
[502–504] and volatile organic compound combustion [505]. Recently,
Ce0.5Zn0.1Co0.1Mg0.1Ni0.1Cu0.1Ox was introduced as a catalyst for cata­
lytic volatile organic compound combustion with a high active oxygen
species [505]. It was shown that this HEO has multi-reactive sites and
can perform the simultaneous combustion of carbon monoxide, pro­
pylene and toluene. The materials acted as a stable catalyst under
thermal and hydrothermal conditions, suggesting the potential of stable
HEOs as alternatives for the CeO2 catalyst.
7.1.3. Ionic conductivity
Although solid-state ion conductivity has been a well-known phe­
nomenon for at least two centuries [506], the phenomenon has become
 S. Akrami et al.
Table 9
Performance of high-entropy oxides for application in Li-ion batteries as anode
materials.
High-entropy Oxide Description
(Co0.2Cu0.2Mg0.2Ni0.2Zn0.2)O [104] Initial specific discharge capacity:
980mAhg− 1, cell reached a capacity of
~600 mAhg− 1 after third cycle and 650
mAhg− 1 after 70 cycles
(Co0.2Cu0.2Mg0.2Ni0.2Zn0.2)O [210] Initial specific discharge capacity: 1585
mAhg− 1 with a reversible capacity of 920
mAhg− 1 at 100 mAg− 1 after 300 cycles
Initial specific capacity: 161− 168 mAhg− 1
(Lix(Co0.2Cu0.2Mg0.2Ni0.2Zn0.2)OFx
Specific discharge capacity: 120 mAhg− 1
[96]
Working potential: 3.4 V vs. Li+/Li
Reversible capacity: 504 mA hg− 1 at 100
mAg− 1 after 300 cycles
Exponential rate capacity: 272 mAhg− 1 at
(Mg0.2Ti0.2Zn0.2Cu0.2Fe0.2)3O4 [156]
2000 mAg− 1
Capacity retention: 96.2 % at 2000 mAg− 1
after 800 cycles
Initial discharge capacity (half-battery):
125.9 mA h g− 1
[(Bi,Na)1/5(La,Li)1/5(Ce,K)1/5Ca1/5Sr1/
Reversible capacity: 120.4 mA h g− 1
5]TiO3 [153]
Delivering retention: 100 % at 1000
mAg− 1 after 300 cycle
Charge-discharge capacity of 1235
Cr,Mg,Fe,Co,Ni-O [533] mAhg− 1 with 90% capacity retention after
200 cycles
(Mg0.2Co0.2Ni0.2Cu0.2Zn0.2O) [114]
Specific capacity: 600 mAhg− 1 with a
Coulombic efficiency close to unit
Initial specific discharge capacity: 890
mAhg− 1, which retained 479 mA hg− 1
Ni,Mg,Cu,Zn,Co oxide [97]
after 600 cycles with a capacity decay of
0.077% per cycle
Initial specific discharge capacity: 446
mAhg− 1, which was maintained at 300
and 256 mAhg− 1 after 50 and 100 cycles,
(Co0.2Cu0.2Mg0.2Ni0.2Zn0.2)O [101]
respectively
Specific energy: 240 Whkg− 1
Power density: 320 Wkg− 1
Initial discharge capacity: 1930 mAhg− 1 at
1000 mAg− 1
(MgCoNiZn)0.65Li0.35O [523]
Stable discharge capacity: 610 mAhg− 1
after 130 cycles at 1000 mAg− 1
Discharge/charge capacity: 1034/680 mA
(FeCoNiCrMn)3O4 [525] h g− 1
Rate capability: 182 mA h g− 1 at 2 Ag− 1
more important in recent decades due to the development of solid-state
fuel cells and batteries. Lithium-ion (Li-ion) batteries, which work based
on the solid-state Li ion conductivity, are considered as one of the most
effective rechargeable batteries for application in portable electronic
devices and electric vehicles [507–510]. Sodium-ion (Na-ion) batteries
are principally similar to Li-ion batteries, but they work based on the Na
ion conductivity. Finding electrolytes with high Li and Na ion
Fig. 26. Enhancement of capacity of Li-ion batteries by using high-entropy oxide anodes. (a) Current versus potential curves for three cycles at the potential sweep
rate of 0.1 mVs− 1, (b) initial three galvanostatic charge-discharge curves (potential versus specific capacity), and (c) capacity for Cr-Mg-Fe-Co-Ni-based high-entropy
oxide anode [533] compared to other anode materials such as silicon, carbon nanotubes, hard carbon and metal oxides [533–544].
24
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Materials Science & Engineering R 146 (2021) 100644
conductivities and developing electrodes with a long cycle life and high
reversible specific capacity are the main challenges in the advancement
of Li-ion and Na-ion batteries [511]. In this section, the research activ­
ities on Li conductivity, Na conductivity and proton (H+) conductivity of
the HEOs are reviewed.
7.1.3.1. Lithium conductivity for lithium-ion batteries. Graphite is a
common anode material for Li-ion batteries [512], while some transition
metal oxides, such as Co3O4 [513], ZnO [513], CuO [514–517], Fe3O4,
[517–520] and Fe2O3 [521,522], are also attracting attention due to
their high capacity and low price. Recently, HEOs were introduced as
potential candidates for the anode of these batteries [156]. Table 9
summarizes the recent attempts to use HEOs in Li-ion batteries [97,101,
114,523–526], indicating that most of the investigated oxides are
Mg-Co-Ni-Cu-Zn-based oxides with the rock-salt structure. The charging
mechanism of the Li-ion batteries using HEOs is complicated and occurs
through the reduction of the transition-metal cations [114,526]. Since
the application of HEOs in Li-ion batteries have a high potential for
future commercialization, the relevant publications are reviewed below.
Berardan et al. [113] introduced the HEOs, (MgCoNiCuZn)1-x-y
GayAxO (A refers to alkali metals such as Li, Na and K), for superionic Li
conductivity and fast-ionic Na conductivity. They reported a Li+ con­
ductivity of >10− 3 Scm− 1 at ambient temperature, which is higher than
the reported conductivity in conventional lithium phosphorus oxy­
nitride by two orders of magnitude [527,528]. They attributed the high
ionic conductivity to oxygen vacancies which are created by lattice
distortion and charge compensation. They suggested that these HEOs are
excellent choices as the electrolytes of batteries.
Osenciat et al. [92] studied the charge compensation mechanisms by
introducing Li+ ions in the superionic conductor (MgCoNiCuZn)1-xLixO.
They demonstrated that for a low concentration of Li+, the charge
compensation occurs by partial Co2+-to-Co3+ oxidation, and for a high
concentration of Li+, the charge compensation occurs by a combination
of Co oxidation and oxygen vacancy formation. Furthermore, they
showed that a high concentration of oxygen vacancies in the HEO has a
negative effect on the Li+ mobility and concluded that reducing the
concentration of the oxygen vacancies by tuning the composition can
lead to an improved Li ion conductivity.
Sarkar et al. [104] commented that HEOs are promising materials for
energy storage in Li-ion batteries. They achieved an initial discharge
capacity of 980 mAhg− 1 for (Co0.2Cu0.2Mg0.2Ni0.2Zn0.2)O with the
rock-salt structure. This capacity is better than those reported using
transition metal oxides [508,529,530]. Furthermore, they investigated
some relevant medium-entropy oxides and confirmed that the presence
of each metal cation influences the electrochemical behavior and cycling
stability. They attributed the good cyclic stability of materials to entropy
stabilization which maintains the rock-salt phase.
Qiu et al. [210] declared that the reason for the remarkable
 S. Akrami et al.
long-term cyclability of (Co0.2Cu0.2Mg0.2Ni0.2Zn0.2)O as an anode ma­
terial is due to a combination of four active elements and an inactive
MgO matrix which are formed after the first discharge process. They
suggested that sluggish diffusion in the HEO is responsible for the cyclic
stability.
Wang et al. [96] introduced multi-anodic and multi-cationic high-­
entropy oxyhalides, Lix(Co0.2Cu0.2Mg0.2Ni0.2Zn0.2)OFx and Nay(Co0.2
Cu0.2Mg0.2Ni0.2Zn0.2)OCly with the rock-salt structure, for Li-ion battery
applications. They used a transition-metal-based HEO and some alkali
metal ions and halides as the precursors to fabricate these oxyhalides.
Since the metal halides have a higher electrochemical potential than
oxides due to the strong ionic character of the metal-fluorine and
metal-chlorine bonds [531,532], they incorporated fluorine and chlo­
rine into the HEO as a cathode material. The oxyhalides could enhance
the operating voltage to 3.4 V vs. Li+/Li. This working potential is higher
than 1.0 V which was reported for the metal-based HEOs [32,101,104,
210].
Chen et al. [156] investigated (Mg0.2Ti0.2Zn0.2Cu0.2Fe0.2)3O4 with
the spinel structure for Li-ion battery application and achieved a
reversible capacity of 504 mA hg− 1. They attributed this good electro­
chemical performance to the material structure, which can buffer the
volumetric changes due to the lithiation/delithiation processes. These
structural changes can provide large sites for the Li storage and accel­
erate the reaction between the electrolyte and charges.
Yan et al. [153] utilized [(Bi,Na)0.2(La,Li)0.2(Ce,K)0.2Ca0.2Sr0.2]TiO3
as the anode for the Li-ion battery and reported an initial discharge
capacity of 125.9 mA hg− 1 with a high cyclic stability. They suggested
that the high cyclic stability and capacity can be due to the stabilization
of a mixed aliovalent cationic structure by entropy as well as due to the
charge compensation mechanism.
Recently, Nguyen et al. [533] synthesized a spinel oxide from Cr, Mg,
Fe, Co and Ni using a hydrothermal technique and investigated its
lithiation-delithiation performance. In this spinel HEO, the inactive
MgO structural pillars, which are used in the rock-salt type HEOs to
enhance the cycling stability, were not utilized. They reported an
excellent charge-discharge capacity of 1235 mAhg− 1 (Fig. 26a and b)
along with retaining a 90 % capacity after 200 cycles. They showed that
the high-rate performance of the electrode is due to the distribution of
the metallic structure and oxygen vacancies leading to high electron and
ion conductivities, respectively. As shown in Fig. 26c, the
charge-discharge capacity of 1235 mAhg− 1 is higher than the capacities
reported using carbon-based or metal-oxide-based anodes [534–544].
The silicon anode has a higher capacity than the HEA anode, but the use
of silicon is limited due to its severe swelling and poor stability during
lithiation. However, compared to silicon, a strong entropy-induced
phase stabilization leads to the high cycling stability of the HEO anodes.
In another study, Wang et al. [545] synthesized lithium-containing
layered delafossite-type HEOs with the general formulation of
Lix(M1M2M3M4M5…Mn)O2 (M = Ni, Co, Mn, Al, Fe, Zn, Cr, Ti, Zr, Cu)
by nebulized spray pyrolysis. They reported reversible Li+ inter­
calation/extraction into/from the HEOs, although the specific capacities
were relatively low compared to the reference data in the literature.
7.1.3.2. Sodium conductivity for sodium-ion batteries. Na-ion batteries
have attracted attention in both academics and industry because of their
low cost and remarkable sources of Na [546]. Oxides are promising for
use as the cathode in Na-ion batteries due to their high structural
compatibility for reversible Na+-(de)intercalation [547]. Researchers
have investigated various NaxTMO2-type oxides to tailor the Na con­
ductivity. Inspired by reports about the high Li conductivity of HEOs,
researchers started to examine the Na conductivity of HEOs.
Zhao et al. [546] studied the electrochemical properties of a
nine-component HEO, NaNi0.12Cu0.12Mg0.12Fe0.15Co0.15Mn0.1Ti0.1Sn0.1
Sb0.04O2, as a cathode material for Na-ion batteries. The material
showed a good cycling stability with an 83 % capacity retention after
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500 cycles. The material exhibited a phase-transition behavior between
the O3 and P3 structures during the charge-discharge process. This
phase transformation is analogous to the phase transformation from the
spinel to rock-salt in (NiFeMnCrCo)xOy, (NiFeMnCrMg)xOy and
(NiFeMnZnMg)xOy during the charge-discharge process of Li-ion batte­
ries [548].
7.1.3.3. Proton conductivity for electrochemical cells. Proton conductivity
defines the movement of H+ in an electrolyte which is normally a solid-state
electrolyte. This phenomenon is of importance in electrochemical cells and
it has become a key issue in recent years due to the development of fuel cells
for hydrogen utilization. Recently, Gazda et al. [549] examined the proton
conductivity of BaZr0.2Sn0.2Ti0.2Hf0.2Ce0.2O3-δ, BaZr0.2Sn0.2Ti0.2Hf0.2
Y0.2O3-δ, BaZr1/7Sn1/7Ti1/7Hf1/7Ce1/7Nb1/7Y1/7O3-δ and BaZr0.15Sn0.15
Ti0.15Hf0.15Ce0.15Nb0.15Y0.10O3-δ with the perovskite structure. They showed
that the materials exhibit a proton conductivity in both dry and wet con­
ditions, while the conductivity improves in the presence of water vapor.
These preliminary results suggest a new research route to employ HEOs for
fuel cells.
7.1.4. Magnetic properties
The magnetic properties of oxides are influenced by their chemical
composition, structure and spin-electronic states [389,550,551]. Eval­
uation of the magnetic properties of HEOs is quite complicated due to
the lattice anisotropy, intrinsic disordered chemistry and structure and
random arrangement of magnetic atoms with diverse electronic/ionic
configurations [152,553]. Diversity of the neighboring ionic
configurations in HEOs leads to a complicated magneto-electronic
free-energy situation and accordingly stabilizes the unconventional
spin-electronic states [552]. The publications about the magnetic
properties of HEOs are next reviewed.
Meisenheimer et al. [389] used (Mg0.2Co0.2Ni0.2Cu0.2Zn0.2)O and
introduced on antiferromagnetic order in the heterostructured
MgO-HEO composite. At the ferromagnetic-antiferromagnetic interface,
exchange coupling was adjusted by tuning the disordering chemistry
and the number of magnetic ions. They reported that the chemical dis­
order was high for the equiatomic concentration of elements and it
further increased by increasing the Co concentration. They showed that
the exchange bias can be improved to values higher than that of con­
ventional permalloy/CoO heterostructures [129] by adjusting the Co
concentration in the HEO.
Zhang et al. [77] examined the magnetic structure of the
(Mg0.2Co0.2Ni0.2Cu0.2Zn0.2)O using direct- and alternating-current
magnetic susceptibility tests and using elastic/inelastic neutron scat­
tering tests. Their results showed that the material has a slow magnetic
transformation with a long-range ordered antiferromagnetic ground
state below the Néel temperature of 113 K. Furthermore, they found that
the magnetic structure includes the ferromagnetic (111) planes with
electron spins antiparallel between two adjacent atomic planes [77].
Jimenez-Segura et al. [98] showed that the rock-salt Mg0.2Co0.2
Ni0.2Cu0.2Zn0.2O synthesized by a solid-state reaction route has a
long-range magnetic ordering at temperatures lower than 120 K in spite
of disordering of the randomly distributed magnetic ions. Furthermore,
they showed that the magnetic ground states are adjustable by compo­
sitional substitutions.
Mao et al. [110] illustrated that the rock-salt Mg0.2Co0.2Ni0.2
Cu0.2Zn0.2O compound fabricated by solution combustion synthesis has
antiferromagnetic long-range-ordered features below the Néel temper­
ature of 106 K and paramagnetic features at ambient temperature. These
features were attributed to super-exchange interactions in the oxide.
Moreover, they showed that the Néel temperature for the HEO is lower
than that for binary oxides (CoO, NiO and CuO) because of disordered
chemistry and large fractions of nonmagnetic atoms in the HEO.
Witte et al. [79] investigated the magnetic properties of several perov­
skites, such as Y(Co0.2Cr0.2Fe0.2Mn0.2Ni0.2)O3, La(Co0.2Cr0.2Fe0.2Mn0.2Ni0.2)
 S. Akrami et al.
Fig. 27. Comparison between magnetic properties of high-entropy oxides and ferromagnetic iron and iron oxide. Magnetic hysteresis loops for (a) BaFe5.83Al1.19
Ti1.08Cr1.12Cu0.78Ga1.03In0.97O19 achieved at 50 and 300 K [200], (b) (Al1/6Co1/6Cr1/6Fe1/6Mn1/6Ni1/6)3O4 achieved at 50, 100, 150 and 300 K [160], (c)
(Cr0.2Fe0.2Mn0.2Co0.2Ni0.2)3O4 (Cr0.2Fe0.2Mn0.2Ni0.2Zn0.2)3O4 and (Cr0.2Fe0.2Mn0.2Co0.2Zn0.2)3O4 achieved at room temperature [161], and (d) Fe, Fe3O4 and
Fe/Fe3O4 achieved at room temperature [553].
O3, Nd(Co0.2Cr0.2Fe0.2Mn0.2Ni0.2)O3, Sm(Co0.2Cr0.2Fe0.2Mn0.2Ni0.2)O3, Gd
(Co0.2Cr0.2Fe0.2Mn0.2Ni0.2)O3 and (Gd0.2La0.2Nd0.2Sm0.2Y0.2)(Co0.2Cr0.2
Fe0.2Mn0.2Ni0.2)O3, by magnetometry and Mössbauer spectroscopy. They
reported a prevailing antiferromagnetic behavior with a small ferromag­
netic participation due to the presence of ferromagnetic clusters within an
antiferromagnetic matrix.
Witte et al. [137] investigated the magnetic properties of the
(Gd0.2La0.2Nd0.2Sm0.2Y0.2)CoO3, (Gd0.2La0.2Nd0.2Sm0.2Y0.2)FeO3 and
(Gd0.2La0.2Nd0.2Sm0.2Y0.2)CrO3 perovskites by X-ray absorption near
edge spectroscopy, magnetometry and Mössbauer spectroscopy. They
found that despite the chemical disordering in the rare-earth sites, there
is a similarity between the magnetic properties of the HEOs and the
magnetic properties of their corresponding binary oxides. However,
they reported some particular magnetic features for the HEOs such as
noncollinearity, spin reorientation transitions as well as large coercive
fields of up to 2 T at ambient temperature.
Vinnik et al. [200] investigated the magnetic properties of
BaFe5.83Al1.19Ti1.08Cr1.12Cu0.78Ga1.03In0.97O19 with the magneto­
plumbite structure. Their results showed that the sample is ferromag­
netic at low temperatures, such as 50 K, and paramagnetic at room
temperature (Fig. 27a). The Curie temperature of the material was as
low as 180.4 K because of dilution of the high magnetic moment cations
by the zero magnetic moment cations. They reported that the high
concentration of high spin cations can improve the paramagnetic
properties of the HEO.
Mao et al. [160] fabricated (Al1/6Co1/6Cr1/6Fe1/6Mn1/6Ni1/6)3O4
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with the spinel structure and investigated its magnetic properties. They
found a long-range ferromagnetic behavior below the Curie temperature
of 248 K due to high super-exchange interactions resulting from the
chemical disordering (Fig. 27b). Mao et al. [161] also investigated the
magnetic properties of (Cr0.2Fe0.2Mn0.2Co0.2Ni0.2)3O4, (Cr0.2Fe0.2Mn0.2
Ni0.2Zn0.2)3O4 and (Cr0.2Fe0.2Mn0.2Co0.2Zn0.2)3O4 with the spinel
structure. Their results showed that the replacement of Zn2+ as a
nonmagnetic ion instead of Co2+ or Ni2+ attenuates the ferromagnetic
ordering (Fig. 27c) and magnetic moments, suggesting a simple
approach to control the magnetic properties of spinel HEOs. A com­
parison between the magnetic behavior of these HEOs and typical
ferromagnetic materials, such as iron and iron oxides (Fig. 27d),
confirmed that the magnetization and Curie temperature in these HEOs
are quite low.
The magnetic materials are used in biomedical applications like cell
separation, contrast agent in magnetic resonance imaging, targeted drug
delivery and thermo-seeds in the hyperthermia treatment of cancer
[202]. Singh et al. [554,555] showed that the ferromagnetic bioactive
41CaO(52-x)SiO24P2O5xFe2O33Na2O can be utilized as thermos-seeds.
They attributed the magnetic properties of these HEOs to the presence
of magnetite (Fe3O4) which is randomly distributed in a matrix.
Shankhwar et al. [202] also synthesized (45-x)SiO2-24.5CaO-24.5­
Na2O-6P2O5xFe2O3 (in wt.%) by the sol-gel method and used it as a
magnetic biomaterial with enhanced magnetic properties.
 S. Akrami et al. Materials Science & Engineering R 146 (2021) 100644

Table 10 electrical resistivity. They reported very low electrical resistivities at

Reported electrical conductivity data of high-entropy oxides. LT and HT refer to ambient temperature which are close to the electrical resistivity of most
low and high temperatures, respectively. metallic alloys, as shown in Table 10. They attributed this feature to the
High-entropy Resistivity Conductivity Conductivity Activation high oxygen vacancy concentration in the structure of the thin films.
Oxide at 300 K ρ Pre- at 300 K σ Energy for Gild et al. [118] investigated the electrical conductivity of eight
(μΩcm) Exponential (Sm− 1) Conductivity Ea fluorite HEOs. All the samples showed lower conductivities than the
Factor (eV)
Y2O3-stabilized ZrO2. Furthermore, they concluded that the addition of
σ0 (Sm− 1)
CaO into the HEOs reduces the conductivity at low temperatures. Since
(AlCrTaTiZr)Ox 1012
the conductivity is influenced by grain size and grain-boundary resis­
[201]
(Co,Cu,Mg,Ni,Zn) 8.039 × 10− 2
0.62 tance [560], they suggested that the small grain size of the fluorites (due
O [95] to slow kinetics of grain growth) is one main reason for the decrease in
814 ± 21 LT
0.31 ± 0.003 the conductivity.
(Co,Cr,Fe,Mn, LT Balcerzak et al. [95] investigated the electrical conductivity of the
Ni)3O4 [157] 0.61 ± 0.005
814 ± 21 HT
HT
rock-salt (Co,Cu,Mg,Ni,Zn)O and showed that the variations in the
0.36 ± 0.002 electrical conductivity versus temperature followed an Arrhenius-type
224 ± 3 LT
(Co,Cr,Fe,Mg, LT plot. They reported that the activation energy for conductivity is 1.01
Mn)3O4 [157] 22,900 ± 355 0.62 ± 0.006 eV for the low-temperature range (478− 641 K) and 0.62 eV for the
HT HT
high-temperature range (990− 1148 K). They achieved the highest
0.38 ± 0.004
(Cr,Fe,Mg,Mn,
2470 ± 214 LT
LT electrical conductivity at 1148 K which was 8.039 × 10− 2 Scm− 1 [95].
Ni)3O4 [157] 137,000 ± 0.62 ± 0.005 Stygar et al. [157] investigated the electrical features of three spinel
8600 HT HT HEOs, (Co,Cr,Fe,Mn,Ni)3O4, (Co,Cr,Fe,Mg,Mn)3O4 and (Cr,Fe,Mg,Mn,
TixFeCoNi-O Ni)3O4, and achieved the σ0 and Ea values which are reported in
30
[208]
Table 10. The materials showed high electrical conductivities at high
TiFeCoNiCu3-O
100 temperature and semiconducting properties at low temperatures.
[208]
Al0.5CrFeCoNiCu- Furthermore, the Seebeck coefficient was in the range of 90–150 μVK− 1,
650
O [208] which is a typical range for semiconductors.
FeCoNiOx [560] 22
CrFeCoNiOx [560] 42
AlFeCoNiOx [560] 18 7.1.5.2. Piezoelectric properties. Typical piezoelectric materials, which
TiFeCoNiOx [560] 35 are utilized for actuators, sensors and microelectronic devices, are based
on lead zirconate titanate (PbTiO3) with the perovskite structure [138].
However, these materials are not environmentally suitable because of
7.1.5. Electrical properties the pollution caused by the toxic Pb. Moreover, the high vapor pressure
High lattice distortion in HEOs due to the presence of multiple cat­ in the sintering process is another problem for using these materials.
ions can significantly influence the electrical properties of these ce­ Some researchers have tried to find new materials, such as Bi0.5Na0.5
ramics. Moreover, differences in the electromagnetic properties of TiO3, as alternatives for the lead zirconate titanate.
contributing cations and their interactions can result in interesting Lin et al. [138] reported (Bi1-x-yNa0.925-x-yLi0.075)0.5BaxSryTiO3 as a
electrical properties. This issue was investigated in various publications, Pb-free piezoelectric ceramic system with the perovskite structure and
as will be discussed below with a focus on the electrical conductivity, investigated its piezoelectric and ferroelectric properties. A comparison
piezoelectric properties and dielectric properties. of their results with pure Bi0.5Na0.5TiO3 confirmed the achievement of a
better piezoelectric coefficient with d33 = 133–193 pCN− 1 for x =
7.1.5.1. Electrical conductivity. In ceramic materials, the electric con­ 0.04− 0.08 and y = 0.02− 0.04.
ductivity and resistivity (inverse of electrical conductivity) are usually of Zachariasz et al. [148] investigated Pb0.94Sr0.06(Zr0.50Ti0.50)0.99
interest to produce insulators particularly at high temperatures, Cr0.01O3 as a modified form of lead zirconate titanate. They commented
although there are activities on exploring conductor ceramics [556, that the material belongs to the ferroelectric-hard materials and can be
557]. Electrical conductivity usually follows the Arrhenius law at used in micromechatronics, resonators, filters and ultrasonic trans­
different temperatures. ducers. The d33 component of the piezoelectric coefficient was 68 pCN− 1
and its dielectric loss was 0.0076 at room temperature.
σ = σ 0 exp(−
Ea
) (21) Bochenek et al. [150] synthesized (Zr0.49Ti0.51)0.94Mn0.014Sb0.02W0.014
KT Ni0.02O3 with the perovskite structure by a calcination method. Their results
demonstrated that the material has a high piezoelectric coefficient of d33 =
where σ, T, σ0 , Ea and K are the electrical conductivity, temperature, pre-
278 pCN− 1, a high dielectric permittivity (1350 at room temperature and
exponential factor, activation energy for electrical conduction and
20,900 at the phase transition temperature of 723 K) and a low dielectric
Boltzmann constant, respectively [558]. Due to the distorted structure of
loss (0.003 at room temperature and 0.140 at 723 K). The low dielectric loss
HEOs and high electron scattering, the introduction of these materials
and high piezoelectric coefficient suggest the potential of this material for
has presented possibilities to produce new insulators with low electrical
modern micromechatronic and microelectronics applications such as
conductivities [559]. The low electrical conductivity of HEOs provides
actuators.
opportunities to fabricate thin film insulators. Table 10 summarizes the
reported data regarding the electrical conductivity of HEOs. The main
findings regarding the electrical conductivity of oxides are reviewed. 7.1.5.3. Dielectric properties. The dielectric properties are important
Lin et al. [201] investigated the electrical resistivity of the (AlCr­ features in designing the electronic devices including capacitors for
TaTiZr)Ox thin film synthesized by DC magnetron sputtering in different energy storage. BaTiO3 is typically used in capacitors. However, for use
concentrations of oxygen and concluded that the electrical resistivity in high-capacitance multilayered ceramic capacitors, there have been
increased by raising the oxygen concentration and reached 1012 μΩ-cm. many attempts to improve its grain-size-dependent dielectric properties.
Tsau et al. [208] fabricated different thin film oxides from TixFeCoNi (x [561]. It was recently shown that HEOs with the rock-salt structure have
= 0, 0.25, 0.5, 0.75 and 1), TiFeCoNiCux (x = 1, 2 and 3) and AlxCr­ high dielectric constants and their properties can be improved by
FeCoNiCu (x = 0.5 and 1) by magnetron sputtering and investigated the changing the concentration of the constituent elements, suggesting that

27
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S. Akrami et al.
Fig. 28. Comparison between dielectric properties of high-entropy oxides and commercial BaTiO3. Relative permittivity (right axis) and dielectric loss (left axis)
versus frequency for (a) Ba(Zr0.2Ti0.2Sn0.2Hf0.2Ta0.2)O3 at room temperature [151], (b) Ba(Zr0.2Ti0.2Sn0.2Hf0.2Nb0.2)O3 at room temperature [151], (c) (Zn,Mg,Ni,Fe,
Cd)Fe2O4 at different temperatures [205] and (d) commercial BaTiO3 at room temperature (processed without, N = 0, and with high-pressure torsion for N = 1 and 5
turns) [561].
HEOs are promising for applications in capacitance-based energy stor­
age tools [88]. Examination of the dielectric properties of HEOs is not
limited to the rock-salt structure as there are attempts to develop
high-entropy dielectric perovskites, as summarized below.
Zhou et al. [151] synthesized several BaTiO3-type perovskites with
the general composition of Ba(Zr0.2Ti0.2Sn0.2Hf0.2Me0.2)O3 (Me = Y, V,
Nb, Ta, Mo, W) using the solid-state reaction. Their results regarding the
dielectric properties demonstrated the high stability of the permittivity
at temperatures from 298 K to 473 K and low dielectric loss of < 0.002 in
the frequency range of 20 Hz to 2 MHz. They mentioned that since a high
entropy can enhance the thermal and electrochemical stability, it can
stabilize the permittivity-loss tangent [104,562]. Despite the superior
permittivity stability, the permittivity of the material was very low
(Fig. 28a and b) which is related to the small grain size and low con­
centration of Ti in the B sites (the B-site sublattice significantly in­
fluences the electric and dielectric permittivity properties [140]).
Furthermore, the materials showed high electrical resistivities and me­
dium breakdown strengths (290− 370 kV/cm) due to the effective
contribution of configurational entropy in enhancement of the charge
carrier scattering [151].
Pu et al. [149] used the thermodynamic calculations to design and
synthesize the HEO, (Na0.2Bi0.2Ba0.2Sr0.2Ca0.2)TiO3, with the perovskite
structure. Investigation of the dielectric properties showed a diffused
phase transmission and frequency dispersion with an energy density of
1.02 Jcm− 3 at 145 kVcm− 1.
Radoń et al. [205] synthesized a high-entropy (Zn,Mg,Ni,Fe,Cd)
Fe2O4 ferrite by the co-precipitation method. They demonstrated that
the high-frequency complex dielectric permittivity is influenced by the
temperature and frequency (Fig. 28c) and its value is comparable to the
one for commercial BaTiO3 (Fig. 28d). They found that the electrical
conductivity of this HEO under an alternating current is related to the
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Materials Science & Engineering R 146 (2021) 100644
quantum mechanical tunneling of electrons and movement of charge
carriers between the Fe2+ and Fe3+ ions. Furthermore, they mentioned
that the highest microwave absorption (reflection loss of < − 25 dB and
shielding effectiveness of < − 50 dB) is achieved at frequencies of
1.9–2.1 GHz for a layer of material with a thickness of 0.8− 1 cm.
Vinnik et al. [141] introduced Na0.30K0.07Ca0.24La0.18Ce0.21TiO3 as a
single-phase perovskite. Their results showed that the loss angle tangent
of BaTiO3 is remarkably less than that of HEO. They reported that the
thermal behavior of the loss angle tangent is different for HEO and
BaTiO3; it continuously increases by raising the temperature for the
HEO, but it shows maximum points for BaTiO3. They also reported that
the permittivity continuously increases with the increasing temperature.
7.1.6. Optical properties
Oxides have a wide range of applications for their optical properties.
The optical properties of the HEOs are of significance not only for future
applications, but also for understanding their electronic structure.
Compared to the other properties already discussed, there have been
rather limited studies about the optical properties of the HEOs. The main
findings about the light absorbance and wavelength conversion of the
HEOs are discussed.
7.1.6.1. Light absorbance. Light absorbance and bandgap are important
features of insulator and semiconductor oxides which significantly in­
fluence their functional properties. Light absorbance not only depends
on the position of the valence and conduction bands, but also on the
lattice distortion and lattice defects (particularly vacancies). Due to the
particular distorted structure of the HEOs, there have been several at­
tempts to examine their light absorbance and bandgap.
Chen et al. [56] investigated the optical bandgap of the AlxCoCr­
CuFeNi (x = 0.5, 1, 2) oxide synthesized by sputtering using different
 S. Akrami et al.
Fig. 29. Dependence of direct (blue marks above 23 eV) and indirect (red
marks below 2.1 eV) bandgaps to pressure in high-entropy oxide
(Ce0.2La0.2Pr0.2Sm0.2Y0.2)O2− δ Bandgaps are smaller than direct bandgap of
3.17 eV and indirect bandgap of 2.76 eV for CeO2 [211] (For interpretation of
the references to colour in this figure legend, the reader is referred to the web
version of this article).
argon to oxygen ratios. They showed that the bandgap changes in the
range of 1− 2 eV and the HEOs have a good infrared transparency
(1000-4000 cm− 1).
Cheng et al. [211] investigated the phase transformation and
bandgap variations of (Ce0.2La0.2Pr0.2Sm0.2Y0.2)O2− δ with the CaF2-type
structure under pressures up to ~35 GPa by in situ synchrotron X-ray
diffraction. They demonstrated that a crystalline-to-amorphous transi­
tion starts at ~16 GPa and completes at ~22 GPa. They found that the
light absorbance and bandgap caused by disordered chemistry and ox­
ygen vacancies are quite sensitive to pressure. They estimated the
bandgap by analyzing the absorption spectra via the Tauc method. They
showed that for pressures less than 16 GPa and before amorphization,
the bandgap of HEO increases by increasing the pressure (Fig. 29). This
behavior is different from most low-entropy oxides in which the
bandgap decreases during compression [563,564]. However, for the
pressures in the range of 16− 22 GPa, the bandgap decreases with the
increasing pressure due to an enhancement in the fraction of the
amorphous phase. For pressures more than 22 GPa, the bandgap again
increases with the increasing pressure. The bandgap of (Ce,La,Pr,Sm,Y)
O under ambient conditions (direct bandgap: 2.06 eV, indirect bandgap:
1.52 eV) is less than the conventional CeO2 material (direct bandgap:
3.17 eV, indirect bandgap: 2.76 eV) due to contribution of the multiple
elements [211].
Edalati et al. [56] examined the light absorbance and bandgap of
TiZrHfNbTaO11 for the photocatalytic activity. As shown in Fig. 23c, the
light absorbance of the material is higher than all binary oxides in this
system such as TiO2, ZrO2, HfO2, Nb2O5 and Ta2O5. The bandgap of HEO
was reported to be 2.9 eV which is smaller than all binary oxides. The
positions of the valence band and conduction band of this material
satisfy the requirement for photocatalytic water splitting.
Sarkar et al. [565] studied the band structure of
(Ce0.2La0.2Pr0.2Sm0.2Y0.2)O2− δ during heat treatment under vacuum, air
and hydrogen atmospheres. They reported a reversible change in the
bandgap from 1.9 eV (under vacuum) to 2.5 eV (under air) and 3.2
(under hydrogen) by changing the heating atmosphere. These changes
were attributed to the oxidation state and f-orbital occupancy of Pr.
Zhang et al. [206] synthesized colorless and transparent
10La2O3-20TiO2-10Nb2O5-20WO3-20ZrO2 ceramics by containerless
solidification through aerodynamic levitation. They reported a refrac­
tive index of 2.22 at 587.6 nm which is influenced by the density, ox­
ygen molar volume and electronic polarizability of oxygen ions. They
commented that these HEOs can be considered as new materials with
better refractive indices and lower wavelength dispersions for applica­
tion in optical windows.
29
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Materials Science & Engineering R 146 (2021) 100644
7.1.6.2. Wavelength conversion. Rare-earth-containing oxides with the
wavelength conversion capability are good candidates to enhance the
efficiency of solar cells [566–573]. The wavelength conversion in these
materials include two independent phenomena; i.e., up-conversion that
can convert long wavelengths of light to shorter ones, and down-shifting
that can convert the short wavelengths of light to longer wavelengths
[573]. Hanioka et al. [574] studied wavelength conversion of Y1-x-yEr
xYbyBaZn3AlO7 which was synthesized by the flux method and reported
down-shifting in the range of 400− 800 nm using an excitation wave­
length of 365 nm. They also found that for excitation at 980 nm,
up-conversion peaks appear at 535, 550 and 661 nm. Furthermore, they
showed that the highest emission intensity for wavelength conversion
can be achieved for the compositions with x = 0.10 and y = 0.20 [574].
7.2. Properties of high-entropy nitrides
Materials which work under extreme situations such as high tem­
perature, corrosive environment or under high wear conditions should
be improved in terms of mechanical properties, thermal stability and
oxidation/corrosion resistance [268]. The surfaces of tools usually
experience the most severe working and environmental conditions, thus,
protective coatings are used to improve the lifetime of tools [268].
Transition metal nitrides, such as TiN, TiAlN and CrAlN [575–578] with
the addition of refractory metals (Zr, Ta, Mo and W), lanthanides (La and
Ce) or Si [579–581], are typically used as coatings in industrial appli­
cations. The binary TiN nitride is the most common coating material due
to its high hardness, low friction coefficient and good adhesion to the
substrates, but it suffers from rapid oxidation at temperatures higher
than 823 K [582,583]. The ternary TiAlN nitride is another conventional
coating system with a high hardness, but it is oxidized at 1073 K [583,
584]. The quarterly TiAlCrN nitride with the addition of Y shows a better
resistance to oxidation [585]. Recent studies confirmed that HENs show
even better mechanical properties, thermal stability, oxidation re­
sistivity and wear resistance in comparison to binary, ternary and
quarterly nitrides [32,136,256,581,586–608].
Nitrides are the first type of ceramics that were developed with the
concept of high-entropy stabilization. In 2004, Chen et al. [48] fabri­
cated nitrides of Fe-Co-Ni-Cr-Cu-Al-Mn and Fe-Co-Ni-Cr-Cu-Al0.5 by
reactive sputtering and investigated the hardness of the HENs as coat­
ings. Since 2004, HENs have been considered as promising materials for
protective coatings and many studies have focused on the mechanical
properties, oxidation resistance and corrosion resistance of these mate­
rials. Besides these common properties, there are other studies about the
application of HENs as diffusion barriers and supercapacitors. These
properties are explained in this section.
7.2.1. Mechanical properties for coating
High hardness is a general requirement of nitrides for use as coatings.
The first publications about HENs in 2004 and 2005 by Chen et al. [48,
54] reported high hardness values for the nitrides of AlxCoCrCuFeNi and
AlCrNiSiTi. A sputtering technique was used to produce thin films and it
was shown that the hardness of AlCrNiSiTi-N is higher than that of
AlxCoCrCuFeNi-N, suggesting its high potential as a coating. Later
studies also showed the high hardness of the nitride of Al-Cr-Mo-Si-Ti
produced by sputtering [393].
Hsieh et al. [609] synthesized a coating of two HENs
(Al23.1Cr30.8Nb7.7Si7.7Ti30.7)N50 and (Al29.1Cr30.8Nb11.2Si7.7Ti21.2)N50 by
reactive magnetron sputtering and investigated the influence of the
substrate bias on the chemical composition, microstructure and me­
chanical properties. The hardness of both HENs increased by increasing
the substrate bias and reached a maximum of 36.1–36.7 GPa. The reason
for increasing the hardness by substrate bias was attributed to a smaller
crystallite size, larger residual stress and denser structure. Huang et al.
[610] employed the Hall-Petch relationship and could determine the
effect of crystallite size on the strengthening of these HENs with a high
accuracy. It was also shown that increasing the intrinsic stress and film
S. Akrami et al. Materials Science & Engineering R 146 (2021) 100644

Table 11
Reported mechanical properties of high-entropy nitrides.
High-Entropy Nitride Hardness (GPa) Indentation Modulus (GPa) Elastic Modulus (GPa) Fracture Toughness (MPam1/2)

Fe-Co-Ni-Cr-Cu-Al-Mn [48] 11
Fe-Co-Ni-Cr-Cu-Al0.5 [48] 11
Al0.5CoCrCuFeNi-N [54] 4.4− 10.4 135− 148
Al2CoCrCuFeNi-N [54] 8.3− 12.4 122.7− 131.3
AlCrNiSiTi-N [54] 12.9− 15.1 141.2− 156.5
(Al29.1Cr30.8Nb11.2Si7.7Ti21.2)Nx [609] 36.7
(AlCrNbSiTiV)N [610] 41 360
(Hf,Ta,Ti,V,Zr)N [268] 30− 34 ~460
(AlCrTiZrHf)N [611] 33.1 347.3
(Cr0.35Al0.25Nb0.12Si0.08V0.20)N [612] 35
(Al0.34Cr0.22Nb0.11Si0.11Ti0.22)50N50 [613] 36
(Ti-Hf-Zr-V-Nb)N [615] 44.3
(TiVZrNbHf)N [617] 60− 65 648
(Al0.5CrFeNiTi0.25)Nx [382] 21.45 253.8
(Zr–Ti-Cr–Nb–Si)N [618] 27 273
(TiZrHfVNbTa)N [619] 42.2
(TiZrNbHfTa)N/MoN [620] 33 315
(Al1.5CrNb0.5Si0.5Ti)Nx [621] 36
AlCoCrNi-N [598] 16.8 243
(FeCoNiCuAlCrV)N [622] 38
(AlMoNbSiTaTiVZr)Nx [623] 37
(AlCrNbSiTiV)N [624] 2493 Hv
(TiZrNbHfTa)N/WN [637] 34 325
(TiVCrZrNbMoHfTaWAlSi)N [625] 34.8
(Al,Ta,Ti,V,Zr)N [638] 30 433 2.4
(AlCrNbSiTiV)N [614] >40
(NbTiAlSiZr)Nx [626] 14.067
(AlCrSiNbZr)Nx [627] 12.3
(AlCrTaTiZr)N [628] 35 350
AlCrTaTiZr-N [629] 32 368
Hf-Nb-Ti-V-Zr-N [630] 18.8 418
(AlCrNbSiTiV)N [631] 37− 41 300− 360
(VAlTiCrMo)Nx [384] 5.731 133.697
(AlCrSiTiZr)100− xNx [639] 16.9 231.5
Al-Cr-Nb-Y-Zr-N [383] 29.6 343
(Al,Cr,Nb,Y,Zr)Nx [632] 27 230− 370
(TiZrHfVNb)N [636] 45
(TiHfZrNbVTa)N [596] 23
CoCrFeMnNi-N [633] >1300 Hv
(Hf0.2Nb0.2Ta0.2Ti0.2Zr0.2)N [616] up to 33 up to 5.2
HfNbTaTiZr-N [634] 27.8 502.6
CrNbTaTiV-N [634] 24.4 476.7
CrHfNbTaTi-N [634] 26.2 488.9
CrHfNbTiZr-N [634] 27.3 488.4
CrHfTaTiZr-N [634] 26.5 465.5
AlCoCrCu0.5FeNi-N [635] 9.8

density are essential to achieve such a high hardness in these HENs,
particularly at high biases.
Kirnbauer et al. [268] showed that the (Hf,Ta,Ti,V,Zr)N film syn­
thesized by reactive magnetron sputtering using the N2 / (Ar + N2) flow
rates of 0.3 and 0.4 have the FCC structure with the high hardness value
of 32.5 ± 0.8 GPa. This hardness was only slightly reduced by annealing
at 1573 K and reached 28.1 ± 1.4 GPa, while the crystal structure
remained stable.
Cui et al. [611] studied the effect of the nitrogen content on the
microstructures and mechanical properties of (AlCrTiZrHf)N. They
demonstrated that the structure of the HEN changes from amorphous to
FCC by increasing the nitrogen gas flow rate, leading to a high hardness
and high elastic modulus of 33.1 GPa and 347.3 GPa, respectively. They
attributed this high hardness to the formation of a saturated nitride
phase with high solid-solution strengthening.
Lin et al. [612] studied the influence of substrate temperature and
bias in the magnetron sputtering system on the hardness of
(Cr0.35Al0.25Nb0.12Si0.08V0.20)N for anti-wear applications. They tuned
the hardness by controlling these two parameters and achieved a high
hardness value of 35 GPa by sputtering at 573 K using a bias of -150 V.
The high hardness was attributed to improved densification and
compressive residual stress.
Shen et al. [613] showed that (Al0.34Cr0.22Nb0.11Si0.11Ti0.22)50N50
has a high hardness of 36 GPa, superior oxidation resistance, good
thermal stability and good adhesion to Ti as an interlayer. Inserts with
this HEN coating and Ti interlayer showed a fine milling behavior in
comparison to conventional inserts coated with TiN and TiAlN, sug­
gesting the high potential of HEN-Ti for protective coating applications.
The good mechanical stability of this HEN was attributed to (i)
high-entropy effect, (ii) severe lattice distortion and (iii) low
grain-boundary energy and low driving force for grain growth [614].
Pogrebnjak et al. [615] studied (TiHfZrVNb)N and found that raising
the bias voltage results in increasing the microhardness due to the
bombardment effect, densification and enhancement of the compressive
stress. They reported a maximum hardness of 44.3 GPa for
Ti0.17Hf0.11Zr0.8V0.6Nb0.9N0.49. They also reported that the tribological
properties of the steel disc effectively improves after deposition of this
superhard nitride.
Moskovskikh et al. [616] showed that the hardness and toughness of
HENs with the FCC structure has close correlation with the valence
electron concentration. They found that the hardness increases to a
maximum value with the increasing valence electron concentration to
8.4 eV and the toughness decreases to a minimum value by raising the
valence electron concentration to 10 [616].
There are some other publications reporting the mechanical prop­
erties of HENs [54,383,384,596,598,614,616–638] which are

30
 S. Akrami et al. Materials Science & Engineering R 146 (2021) 100644

Table 12
Mechanical and thermal properties of high-entropy carbides.
High-Entropy Carbide Hardness Elastic Modulus Fracture Toughness Strength (MPa) Thermal Conductivity Thermal Diffusivity
(GPa) (GPa) (MPam1/2) (Wm− 1 K− 1) (mm2s− 1)

(TiAlCrNbY)C [59] 22.6 ± 1.2

(Hf, Zr, Ti, Ta, Nb)C [690] 27.5
(CuSiTiYZr)C [719] 29.5
(CrCuNbTiY)C [720] 29
(Ti0.2Zr0.2Hf0.2Nb0.2Ta0.2)C [275] 32 ± 2 445
(Ti0.2Hf0.2V0.2Nb0.2Ta0.2)C [275] 29 505
(Ti0.2V0.2Nb0.2Ta0.2W0.2)C [275] 28 485
(Ti0.2Zr0.2Hf0.2Ta0.2W0.2)C [275] 33 475
(Ti0.2Hf0.2Nb0.2Ta0.2W0.2)C [275] 31 485
(V0.2Nb0.2Ta0.2Mo0.2W0.2)C [275] 27 585
(Ti0.2Hf0.2Nb0.2Ta0.2Mo0.2)C [275] 27 480
(TiZrNbTaMo)C [682] 31.3 ± 2.5 3.28 ± 0.12
B4(HfMo2TaTi)C + SiC [260] 35.4 472.4
Hf0.2Ta0.2Ti0.2Nb0.2Zr0.2C [283] 25.7 ± 3.5 473 ± 37 5.6 ± 0.1
(Zr0.2Hf0.2Ti0.2Nb0.2Ta0.2)C [722] 3.45 0.39 0.74
compressive
(Ti0.2Zr0.2Hf0.2Nb0.2Ta0.2)C [712] 21.9 ± 0.4 4.51 ± 0.61 332 ± 24
(Hf0.2Zr0.2Ta0.2Nb0.2Ti0.2)C [713] 17.07 ± 0.54 5.9 ± 0.7 400 ± 27
bending
(Hf, Zr, Ti, Ta, Nb)C [340] 24.4 ± 0.5 452 ± 6
(Ti, Zr, Nb, Ta, Hf)C [714] 31.9 ± 3.1 379.2 ± 25.9
(Hf, Zr, Ti, Ta, Nb)C [261] 18.8
(Hf, Zr, Ti, Ta, Nb)C [313] 15
(Ti0.2Zr0.2Hf0.2Nb0.2Ta0.2)C + 20% 25 ± 0.8 5.24 ± 0.41 554 ± 73
SiC [712]
(VNbTaMoW)C [715] 9.2
Hf0.2Ta0.2Ti0.2Nb0.2Mo0.2C [283] 23.8 ± 2.7 544 ± 48 5.9 ± 0.2
(TiZrNbTaHf)C [267] 32
(Zr0.25Nb0.25Ti0.25V0.25)C [258] 22.5
FeCoCrNiMn-C [724] 857 tensile
TiC0.4/WC/0.5 Mo2C [725] 23.7 6.2
(Hf-Ta-Zr-Nb)C [686] 36.1 ± 1.6 598 ± 15
TiZrNbC [687] 2.9 496 ± 44
flexural
(Hf,Zr,Ti,Ta,Nb)C [717] 25.0 ± 1.0 450 3.5 ± 0.3
(Ti,Zr,Hf,V,Nb,Ta,Cr,Mo)C [718] 41.2 ± 1.0

summarized in Table 11. As can be seen, even a hardness value of 65 GPa
was reported for (TiVZrNbHf)N [617], which suggests that this new
class of materials have high potential to be used as superhard materials.
7.2.2. Oxidation resistance
Oxidation resistance, as an important property for developing a
protective coating, was investigated for several HENs. Shen et al. [640]
studied the oxidation behavior of (Al0.34Cr0.22Nb0.11Si0.11Ti0.22)50N50
and reported a high oxidation resistance up to 1573 K. The weight gain
was only 0.015 mgcm− 2 after a 50-h oxidation at 1573 K. They showed
that there are eight oxide layers on the surface with various composi­
tions. The high oxidation resistance of this HEN was attributed to a thick
Al2O3 surface layer and an internal Si-rich amorphous-like network.
Pogrebnjak et al. [615] studied the oxidation behavior and tribo­
logical features of (TiHfZrVNb)N films synthesized by
cathodic-arc-vapor deposition. The oxidation of HEN started at the
relatively low temperature of 873 K by formation of rutile TiO2 and
other MTiO4-type oxides.
Hsieh et al. [609] studied the oxidation resistance of two HEN
coatings (Al29.1Cr30.8Nb11.2Si7.7Ti21.2)N50 and Al23.1Cr30.8Nb7.7
Si7.7Ti30.7)N50 by oxidation at 1173 K for 2 h in air. The thickness of the
oxide layer was as thin as 100 ± 12 nm for (Al23.1Cr30.8Nb7.7Si7.7Ti30.7)
N50 and 80 ± 7 nm for (Al29.1Cr30.8Nb11.2Si7.7Ti21.2)N50. The reason for
the better oxidation resistance of (Al29.1Cr30.8Nb11.2Si7.7Ti21.2)N50 was
attributed to its higher Al/Ti ratio (Al2O3 layer is more protective than
TiO2).
7.2.3. Corrosion resistance
Corrosion resistance in another important requirement for protective
nitride coatings particularly when they are utilized in severe
environments such as sea water, acidic rainwater or acidic solutions
[639,641–644]. TiN coatings have fine anti-corrosion properties due to
the creation of a nitrogen-rich layer on the surface [643,645]. The
corrosion resistance of HENs was evaluated in a few studies, which
suggested the reasonable resistance of these materials.
Hsueh et al. [639] studied the influence of the nitrogen fraction and
bias on the corrosion resistance of (AlCrSiTiZr)100− xNx films. They
investigated the corrosion behavior by anodic polarization analysis in a
0.1 M H2SO4 aqueous solution under ambient conditions. They illus­
trated that the corrosion resistance can be significantly improved by
tuning the nitrogen content and increasing the substrate bias due to
changes in the film composition, film structure, film density and
coat-substrate bonding.
Fieandt et al. [632] also investigated the corrosion behavior of (Al,
Cr,Nb,Y,Zr)N and demonstrated its better corrosion resistance in com­
parison to a commercially hyper-duplex stainless steel and a ternary
(Nb,Zr)N thin film.
7.2.4. Diffusion resistance for barriers
The need for circuit density and resistance-capacitance delay is
growing by the fast improvement of integrated circuits in microelec­
tronics [646,647]. Cu on a Si substrate is usually used to decrease the
resistance-capacitance delay problem [648–651]. However, due to the
high diffusivity of Cu in Si, this interconnection can produce copper
silicides and damage the microelectronic devices [652–654]. To avoid
the penetration of Cu in Si, an appropriate diffusion barrier with high
thermal stability, high electrical resistivity and strong interface bonding
is required [655]. HENs were evaluated as a diffusion barrier in a few
studies.
Chang et al. [656] investigated AlCrTaTiZrN as a diffusion barrier in

31
­
S. Akrami et al.
Table 13
Oxidation behavior of high-entropy carbides. ΔW and A refer to the weight
change and surface area, respectively.
High-Entropy Carbide Oxidation Behavior
(ΔW/A)2 ≈ 2300 mg2 cm− 4 after 60 min at
1773 K
(Hf0.2Zr0.2Ta0.2Nb0.2Ti0.2)C [304]
(ΔW/A)2 ≈ 170 mg2 cm− 4 after 120 min at
1573 K
(ΔW/A)2 ≈ 1800 mg2 cm− 4 after 120 min at
1273 K
(Hf0.2Zr0.2Ta0.2Nb0.2Ti0.2)C [303]
(ΔW/A)2 ≈ 100 mg2 cm− 4 after 120 min at
1073 K
(Ti,Zr,Hf,Nb,Ta)C [726]
21.25 % weight gain at 369 K
22.5 % weight gain at 676 K
(ΔW/A)2 ≈ 145 mg2 cm− 4 after 120 min at
(Hf0.2Ta0.2Zr0.2Ti0.2Nb0.2)C-xSiC 1773 K with 10 vol% SiC
[322] (ΔW/A)2 ≈ 37 mg2 cm− 4 after 120 min at 1573
K with 30 vol% SiC
(ΔW/A)2 ≈ 22 mg2 cm− 4 after 70 min at 1273 K
(Zr,Ti,Hf,Nb,Ta)C [322]
(ΔW/A)2 ≈ 7 mg2 cm− 4 after 70 min at 1473 K
the temperature range of 973− 1173 K. The material was thermally
stable at 1173 K and showed a low electrical resistance and high diffu­
sion resistance. The high thermal stability and superior diffusion resis­
tance was attributed to a severe lattice distortion that is created by the
addition of multi-principal elements. They found that the material has
features of a nanocomposite covered by an amorphous phase and
without the presence of grain boundaries.
Li et al. [385] evaluated the thermal stability of amorphous (AlCr­
TaTiZrMo)N as a single-layer barrier material for a Cu and Si intercon­
nection at 873 K. Their investigation demonstrated that the layer has a
suitable thermal stability for at least 7 h and does not have any large
holes or cracks on the surface. The material showed a good interface
adhesion to Cu and Si with a high diffusion resistance. They attributed
the good performance of the material as a diffusion barrier to its
amorphous structure and high-entropy-induced slow diffusion.
7.2.5. Supercapacity for electronic supercapacitors
Metal nitrides are used in supercapacitors for energy storage [657,
658]. Jin et al. [372] synthesized an HEN from five transition-metals (V,
Cr, Nb, Mo, Zr) by a soft urea method combined with mechanochemical
processing and examined its supercapacity. The materials showed
appreciable properties for application as a supercapacitor; a specific
capacity of 78 Fg− 1 in 1 M KOH at the scanning speed of 100 mVs− 1.
They demonstrated that the capacitance of this HEN is comparable or
even better than previously introduced metal nitride capacitors [657,
658]. For example, the capacity for the conventional VN@C is 46.9 Fg− 1
which is lower than the value of 78 Fg− 1 achieved for this HEN under the
same experimental conditions [657].
7.2.6. Photothermal conversion for solar selective absorber coatings
Sunlight absorption by photothermal conversion has attracted
attention in different research fields particularly in the solar power
systems [659]. There have been significant attempts to find appropriate
solar selective absorber coatings with a high efficiency from oxides and
nitrides. Two main parameters influence the efficiency of solar absorber
coatings; i.e., solar absorbance (α) and thermal emittance (ε). A high
ratio of solar absorbance to thermal emittance defines a good spectral
selectivity (α/ε) and is desirable for solar selective absorbance coatings.
He et al. [659] used the AlCrTaTiZrN compound for solar selective
absorbance. This HEN showed a high solar absorbance (α = 0.965) and
low thermal emittance (ε = 0.086) with a high spectral selectivity. The
HEN could keep its crystal stability and good spectral selectivity even
after annealing at 873 K for 10 h, suggesting the high potential of
high-entropy ceramics for application in solar power systems. A few
other studies also confirmed the potential of HENs for solar selective
absorbance [660–663].
32
Materials Science & Engineering R 146 (2021) 100644
7.3. Properties of high-entropy carbides
HECs were introduced in 2010 by Braic et al. [59], who synthesized
the thin film of (TiAlCrNbY)C by reactive magnetron sputtering. In the
following years, HECs were studied for various possible applications
[664–676] including protective coatings and ultrahigh-temperature
ceramics. Ultrahigh-temperature ceramics, such as Zr2B [677,678],
HfB2 [679] and TaC [680,681], are materials which can withstand a
load under high temperatures due to their high thermal stability, high
hardness, high mechanical strength and good creep and wear resistance
[260]. These ultrahigh-temperature ceramics particularly in the form of
transition metal carbides with the SiC addition are widely used as cut­
ting tools and high-temperature tribological-resistant parts [682–685].
Single-phase HECs are basically attractive for these applications because
of their high hardness, small thermal conductivity and good creep and
oxidation resistivity at high temperatures [267,275,313,314,686–691].
In addition to coating- and ultrahigh-temperature-related properties, the
biocompatibility [690,692], magnetic properties [693] and electrical
properties [212,259] of HECs were also investigated in recent years.
HECs are currently the second most investigated high-entropy ceramics
due to their attractive properties [234,694–711]. The major reports
about the properties of HECs are reviewed in this section.
7.3.1. Mechanical and thermal properties
Mechanical and thermal properties of HECs are summarized in
Table 12. These properties have been of interest particularly because of
the potential application of HECs as protective coating and ultrahigh-
temperature ceramics [258,261,267,283,313,340,686,687,712–718].
In 2010, Braic et al. [59] deposited the (TiAlCrNbY)C films as a pro­
tective coating by reactive magnetron sputtering. In the following years,
they extended their study to (TiZrNbHfTa)C [690], (CuSiTiYZr)C [719]
and (CrCuNbTiY)C [720] and compared their materials with TiN and
TiC as two conventional coating materials. They found that these HECs
have a higher hardness and superior wear resistance performance
compared with TiN and TiC. Furthermore, they showed that a hardness
of 31 GPa can be achieved by increasing the carbon fraction in the HECs.
They investigated the effect of substrate temperature on mechanical
properties and demonstrated that the hardness and wear resistance are
improved by increasing the substrate temperature.
Harrington et al. [275] studied the mechanical properties of seven
single-phase HECs with the rock-salt structure. All the investigated
high-entropy carbides demonstrated an enhanced hardness compared to
the binary carbides. Furthermore, they showed that the hardness of the
HECs decreased and their elastic modulus increased with the increasing
valence electron concentration in the range of 8.4–9.4, confirming the
strong correlation of hardness with the electronic structure of the HECs.
Their DFT calculations suggested that the random distribution of ele­
ments (and not entropy) is a key factor for enhancing the mechanical
properties.
Wang et al. [682] employed the nanoindentation method and re­
ported high hardness values of 25.3–31.3 GPa for the dense (TiZrNb­
TaMo)C synthesized by two-step hot pressing. These hardness values are
higher compared to typical carbides due to the composition effect and
small grain sizes. However, this HEC showed the low fracture toughness
of 3.28 MPam1/2 due to lack of effective toughening mechanisms. A
comparison between the hardness of this HEC with the reported hard­
ness of (HfZrTaNbTi)C (15–18.8 GPa [261,313]) suggests that Mo plays
a critical role in hardening of (TiZrNbTaMo)C through the grain
refinment.
Zhang et al. [260] synthesized B4(HfMo2TaTi)C + SiC as an
ultrahigh-temperature ceramic by the pulsed current processing
method. They showed that the theoretical hardness value for this HEC
(23.2 GPa) is 48 % lower than the experimental value (35.4 GP) due to
the elevated solution hardening effect [686]. They investigated the
oxidation resistance at 1173 K after 50 h and reported less than a 1 %
weight loss. Furthermore, they demonstrated that the addition of SiC
S. Akrami et al. Materials Science & Engineering R 146 (2021) 100644

Table 14
Mechanical and thermal properties of high-entropy borides.
High-Entropy Boride Sintering Sintering Hardness Elastic Strength Fracture Thermal
1
Temperature (K) Time (min) (GPa) Modulus (MPa) Toughness Conductivity (Wm−
(GPa) (MPam1/2) K− 1)

(Hf0.2Zr0.2Ta0.2Nb0.2Ti0.2)B2 [61] 2273 5 17.5 ± 1.2

(Hf0.2Zr0.2Ta0.2Mo0.2Ti0.2) B2 [61] 2273 5 19.1 ± 1.8
(Hf0.2Zr0.2Mo0.2Nb0.2Ti0.2)B2 [61] 2273 5 21.9 ± 1.7
(Hf0.2Mo0.2Ta0.2Nb0.2Ti0.2)B2 [61] 2273 5 22.5 ± 1.7
(Mo0.2Zr0.2Ta0.2Nb0.2Ti0.2)B2 [61] 2273 5 23.7 ± 1.7
(Hf0.2Zr0.2Ta0.2Cr0.2Ti0.2)B2 [61] 2273 5 21.0 ± 2.8
(Hf0.2Mo0.2Ta0.2Nb0.2Ti0.2)B2 [347] 1223 20 22.5 ± 1.7
(Hf0.2Zr0.2Ti0.2Ta0.2Mo0.2)B2 [333] 2273 5 24.9 ± 1.0 15.2 ± 3.5
(Hf0.2Zr0.2Ti0.2Ta0.2Cr0.2)B2 [333] 2273 5 24.9 ± 1.0 12.6 ± 2.5
(Hf0.2Zr0.2Ti0.2Mo0.2W0.2)B2 [333] 2273 5 29.4 ± 1.7
(Hf0.2Zr0.2Ta0.2Nb0.2Ti0.2) B2 [334] 2273 10 21.7 ± 1.1 4.06 ± 0.35
(Hf0.2Zr0.2Mo0.2Nb0.2Ti0.2)B2 [334] 2273 10 26.3 ± 1.8 3.64 ± 0.36
(Hf0.2Mo0.2Ta0.2Nb0.2Ti0.2) B2 [334] 2273 10 27.0 ± 0.4 4.47 ± 0.40
(Ti0.2Hf0.2Zr0.2Nb0.2Ta0.2)B2 [338] 2273 5 25.6 ± 0.8 500 2.83 ± 0.15
(Ti0.2Hf0.2Zr0.2Nb0.2Ta0.2)B2 [338] 2323 5 26.8 ± 1.8 527
(Hf0.2Zr0.2Ta0.2Cr0.2Ti0.2)B2 [586] 2273 10 28.3 ± 1.6
(Hf0.2Mo0.2Zr0.2Nb0.2Ti0.2)B2 [586] 2273 10 26.3 ± 0.7
(Hf0.2Mo0.2Ta0.2Nb0.2Ti0.2)B2 [586] 2273 10 25.9 ± 1.1
(Hf0.2Zr0.2Ta0.2Cr0.2Ti0.2)B2 [763] 2273 10 29
(Zr0.2Ta0.2Ti0.2Nb0.2Hf0.2)B2 [331] 2273 10 16.4 ± 0.5
(Zr0.2W0.2Ti0.2Mo0.2Hf0.2)B2 [331] 2273 10 27.7 ± 1.1
(Hf0.2Zr0.2Ti0.2Ta0.2Nb0.2)B2 [333] 2273 5 20.5 ± 1.0 24.8 ± 5.1
(Ti0.2Zr0.2Hf0.2Mo0.2W0.2)B2 [300] 2273 10 26.0 ± 1.5
(Ti0.2Ta0.2Cr0.2Mo0.2W0.2)B2 [300] 2273 10 23.7 ± 1.3
(Zr0.2Hf0.2Nb0.2Ta0.2W0.2)B2 [300] 2273 10 26.7 ± 1.1
(Zr0.225Hf0.225Ta0.225Mo0.225W0.1)B2 2273 10 27.5 ± 1.1
[300]
(Ti0.2Zr0.2Hf0.2Nb0.2Ta0.2)B2 [300] 2273 10 20.9 ± 1.1
(Ti0.2Zr0.2Nb0.2Ta0.2Mo0.2)B2 [300] 2273 10 24.9 ± 1.3
(Zr0.2Ta0.2Ti0.2Nb0.2Hf0.2)B2 [764] 2273 5 25.3 ± 0.6 544 ± 8
(Zr0.2Hf0.2Ti0.2Nb0.2Ta0.2)B2 [341] 3.93 0.51
compressive
(Zr0.23Ti0.20Hf0.19V0.14Ta0.24)B2 [387] 47.2 ± 1.8 540 ± 17
(Ti0.2Zr0.2Hf0.2Nb0.2Ta0.2)B2 [311] 1173 10 22.5 505 3
(Ti0.2Zr0.2Hf0.2Nb0.2Ta0.2)B2-20 vol% 1173 10 23 460 4.7
SiC [311]
(Ti0.2Zr0.2Hf0.2Nb0.2Ta0.2)B2 [744] 23.7 ± 0.7 448 339 ± 17 3.81 ± 0.40
bending
(Ti0.2Zr0.2Hf0.2Nb0.2Ta0.2)B2-20 vol% 24.8 ± 1.2 419 447 ± 45 4.85 ± 0.33
SiC [744] bending
(Ti0.2Zr0.2Hf0.2Nb0.2Ta0.2)B2 [745] 22.7 ± 1.9
(Hf0.2,Zr0.2,Ti0.2,Ta0.2,Cr0.2)B2 [746] 22.6
(Y0.2Yb0.2Sm0.2Nd0.2Eu0.2)B6 [747] 12.71
compressive
(Y0.2Yb0.2Sm0.2Nd0.2Eu0.2)B6 [747] 31.59
compressive
(Y0.2Nd0.2Sm0.2Gd0.2Tb0.2)B4 [748] 13− 15
(Hf0.2Zr0.2Mo0.2Nb0.2Ti0.2)B2–20 vol% 29.0 ± 1.3 3.80 ± 0.33
SiC [749]
(Hf0.2Mo0.2Ta0.2Nb0.2Ti0.2)B2–20 vol% 28.1 ± 0.9 4.25 ± 0.37
SiC [749]
(V0.2Cr0.2Nb0.2Mo0.2Ta0.2)3B4 [750] 18.6 ± 1.2
(V0.2Cr0.2Nb0.2Ta0.2W0.2)3B4 [750] 19.8 ± 0.9

improves the structure and oxidation resistivity of the material at
elevated temperatures. The reason for the remarkable oxidation resis­
tance of this HEC + SiC was attributed to the formation of SiO2 on the
sample surface as a protection layer [721].
Moskovskikh et al. [283] studied the mechanical properties and
thermal conductivity of two HECs, Hf0.2Ta0.2Ti0.2Nb0.2Mo0.2C and
Hf0.2Ta0.2Ti0.2Nb0.2Zr0.2C, synthesized by ball milling and spark plasma
sintering. They achieved the hardness, elastic modulus and thermal
conductivity of 25.7 ± 3.5 GPa, 473 ± 37 GPa and 5.6 ± 0.1 Wm− 1 K− 1
for Hf0.2Ta0.2Ti0.2Nb0.2Zr0.2C and 23.8 ± 2.7 GPa, 544 ± 48 GPa and 5.9
± 0.2 Wm− 1 K− 1 for Hf0.2Ta0.2Ti0.2Nb0.2Mo0.2C, respectively. These
values are superior compared to many other reported results [3,45,70,
313]. They suggested that the presence of particles of oxides, such as
HfO2, is one of the main reasons for the hardening of these HECs [682].
Chen et al. [722] synthesized porous (Zr0.2Hf0.2Ti0.2Nb0.2Ta0.2)C by
ball milling and reported a good combination of properties as an
ultrahigh-temperature ceramic such as a thermal conductivity of 0.39
Wm− 1 K− 1, a thermal diffusivity of 0.74 mm2s− 1 and a high compressive
strength of 3.45 MPa with a good thermal stability.
Rost et al. [723,724] showed that the thermal conductivity of the
HECs decreased by enhancing the carbon stoichiometry in the compo­
nent. They reported that when the carbon content increases, the struc­
ture of the HECs changes from a metal-like state with metallic bonds to a
ceramic-like state with covalent bonds. They found that the role of the
electronic contribution on the thermal conductivity is reduced and the
role of phonon scattering on the thermal conductivity is enhanced by the
formation of such a ceramic-like structure.
7.3.2. Oxidation resistance
As summarized in Table 13, the oxidation resistance of the HECs

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Fig. 30. Reversible room-temperature hydrogen storage in TiZrMnCrFeNi-TiZrMnCrFeNiH6 system with major C14 Laves phase structure. (a) Crystal orientation
mapping achieved by electron backscatter diffraction, (b) crystal phase mapping and (c) cyclic pressure-composition-temperature isotherms for hydrogen absorption/
desorption at room temperature [271].

Fig. 31. High electrocatalytic activity and low overpotential of high-entropy phosphides for water splitting. (a) Electrocatalytic polarization curves (current density
versus potential) for water splitting on high-entropy phosphide Co-Cr-Fe-Mn-Ni-P compared to binary phosphides and Pt/C‖IrO2 electrocatalyst (dotted line) for
hydrogen evolution (left) and oxygen evolution (right), and (b) overpotential for hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) compared
to binary phosphides and Pt/C and IrO2 electrocatalysts at the current density of 10 mAcm− 2 [72].

based on the Ti-Zr-Hf-Nb-Ta system was investigated in several studies. In these equations, A is the surface area, ΔW is the weight change, t is
The oxidation behavior of metal carbides usually follows two behaviors: the time and kl and kp are the slope of the linear and parabolic re­
(i) linear behavior and fast oxidation as in Eq. (22), and (ii) parabolic lationships, respectively [304]. Ye et al. [303] evaluated the oxidation
behavior and slower oxidation as in Eq. (23) [304]. behavior of (Ti,Zr,Hf,Nb,Ta)C, because this HEC was reported to have a
( ) good oxidation resistance [725,726]. They demonstrated that the
ΔW
= k1 t (22) oxidation behavior of this HEC at 1073− 1473 K follows a parabolic rate
A
law. They also found that the oxidation rate first increases by raising the
ΔW 2 temperature from 1073 to 1273 K, but it decreases by increasing the
( ) = kp t (23) temperature from 1273 to 1473 K. In another study [304], they
A
increased the oxidation temperature to 1573–1673 K and confirmed that

34
S. Akrami et al.
Table 15
Mechanical properties of high-entropy carbonitrides.
High-Entropy Carbonitride Nanohardness Elastic Modulus
(GPa) (GPa)
HfNbTaTiZr(CN)x [634] 32 557.9
CrNbTaTiV(CN)x [634] 30 518.2
CrHfNbTaTi(CN)x [634] 29.9 564.5
CrHfNbTiZr(CN)x [634] 30.4 531.9
CrHfTaTiZr(CN)x [634] 29.7 550
(Hf0.2Zr0.2Ta0.2Nb0.2Ti0.2)(N0.5C0.5) 33.4 ± 0.5 572 ± 7
[835]
the HEC shows a good oxidation resistance, but follows a parabolic law
in this temperature range (the material was entirely oxidized at 1773 K
within 1 h). The good oxidation resistance of this HEC was attributed to
the formation of different oxides within different layers of the surface
[303].
Tan et al. [323] investigated the oxidation behavior of the bulk
high-entropy (Zr,Ti,Hf,Nb,Ta)C at 1473 K in an atmosphere with a 90 %
relative water humidity to clarify the possible application of the material
in nuclear reactors. This material illustrated a good oxidation resistance
under this condition with a parabolic rate behavior and a kp value two
times lower than that of ZrC.
Wang et al. [322] studied the oxidation resistance of
(Hf0.2Zr0.2Ta0.2Nb0.2Ti0.2)C mixed with different amounts of SiC (10, 20
and 30 vol%) in the temperature range of 1573− 1773 K. They found
that the addition of SiC improves the oxidation resistivity of material
due to the formation of HfZrSiO4 and HfZrTiO4 as protective layers. The
sample with a 20 vol% SiC showed the best oxidation resistance. They
illustrated that the SiC addition cannot affect the oxidation mechanism,
but it postpones the outward diffusion of other elements. They com­
mented that the rate of the oxidation process is controlled by the out­
ward diffusion of Ti in the samples mixed with SiC.
7.3.3. Biocompatibility
Biocompatibility is another property which was investigated for
HECs. There are some hard ceramic coatings which demonstrate an
excellent biocompatibility including nitrides (TiN, ZrN, NbN, TiSiN and
TiHfN) [727,728], carbides (TiC, ZrC, NbC and TaC) [729,730] and
carbonitrides (TiCN and ZrCN) [731–733]. The superior properties of
HECs such as high hardness, excellent stability, good corrosion and wear
resistivity suggest them as potential candidates for coatings in biomed­
ical applications.
Braic et al. [690,692] investigated the mechanical properties,
tribological properties, corrosion resistance and biocompatibility of
(TiNbZrTaHf)C and concluded that this HEC can be suitable for
biocompatibility applications. In another research study from this
group, Vladescu et al. [388] tried to replace Ti and Ta by Si for two main
reasons; i.e., (i) the addition of Si to binary and ternary carbides can
enhance the mechanical, anticorrosive and tribological properties [734,
735], and (ii) the presence of Si in various biomaterials shows a positive
effect on the proliferation and differentiation of human osteoblast-like
cells and positive effect on osseointegration of metallic implants [736,
737]. They performed biocompatibility tests by measuring the cell
viability and cell attachment to the coated surface and confirmed that
the substitution of Si instead of Ta enhanced the biocompatibility of
(TiZrNbSiHf)C [388].
7.3.4. Electromagnetic wave absorption
Electromagnetic wave absorbing materials are widely used in the
communication and information processing systems to prevent the
leakage of information and to avoid damage to the environment and
humans body [738]. Due to the rapid reduction of the size of electronic
devices in the communication and information processing systems, there
are significant attempts to discover new ceramics or carbon-based
nanosheets, nanowires or nanofibers with a high electromagnetic
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Materials Science & Engineering R 146 (2021) 100644
wave absorption efficiency and good stability.
Recently, Zhou et al. [738] investigated an HEC
(Ti0.2Zr0.2Hf0.2Nb0.2Ta0.2)C for electromagnetic wave absorption and
compared its performance to related monocarbides. They examined the
medium reflection loss and effective absorption bandwidth as two main
parameters influencing the electromagnetic wave absorption. They
found that compared to HfC and TaC with superior absorptions, the
medium reflection loss and effective absorption bandwidth of the HEC
are not very high. However, they concluded that it is still possible to
design new high-entropy ceramics with a high electromagnetic wave
absorbance through dielectric/magnetic loss coupling by tuning the
crystal-field splitting energy of the d orbitals.
7.4. Properties of high-entropy borides
Borides, such as ZrB2, HfB2 and TaB2, are promising ultrahigh-
temperature ceramics due to their high melting temperature and good
thermal/mechanical/chemical stabilities. These materials are utilized as
structural components which can work at ultrahigh temperatures [739,
740], but their thermomechanical properties and stability should be
improved in extreme situations [741,742]. Recently, the high-entropy
ultrahigh-temperature ceramics have been considered as a solution to
overcome the limitation of typical ceramics at ultrahigh temperatures
[313]. Among all these high-entropy ceramics, HEBs are considered as a
novel family of ceramics for such applications [309,334,743]. There­
fore, most of the studies about HEBs focused on the thermomechanical
properties and oxidation resistance, although the electromagnetic
properties and thermal conductivity of these materials as insulator
coatings were also investigated [311,387,744–762]. Table 14 summa­
rizes the reported mechanical and thermal properties of the HEBs.
7.4.1. Mechanical properties
The mechanical properties and particularly the hardness of HEBs
have been of interest since their introduction. In one of the earliest
studies, Gild et al. [61] showed that the hardness of HEBs synthesized by
ball milling and spark plasma sintering is better than binary borides.
They suggested that ball milling leads to the formation of pores and
oxides in the structure, which can negatively affect the hardness. Tal­
larita et al. [347] modified the synthesis route to a two-step self-­
propagating high-temperature synthesis and spark plasma sintering at
2223 K and achieved hardness values similar to those reported by Gild
et al. [61]. Gild et al. [333] later synthesized HEBs by borothermal
reduction and spark plasma sintering. They demonstrated that the
samples fabricated by these two methods have a better hardness
compared to samples produced by ball milling and spark plasma sin­
tering. They reported a maximum hardness of 29.4 ± 1.7 GPa for
(Hf0.2Zr0.2Ti0.2Mo0.2W0.2)B2. There are several other efforts by Gild et al.
[309] and others [334,338,347] to modify the synthesis routes in order
to improve the properties of HEBs.
Zhang et al. [586] showed that increasing the sintering time and
temperature during spark plasma sintering can improve the relative
density and mechanical properties due to completion of the reactions. In
another study [763], they produced a textured (Hf0.2Zr0.2Ta0.2Cr0.2Ti0.2)
B2 using spark plasma sintering of a powder prepared by bor­
ocarbothermal reduction. They showed that the hardness for their ma­
terial was ~29 GPa regardless of the texture, but the fracture toughness
was enhanced by the formation of elongated grains [763]. Zhang et al.
[331] also used the borothermal reduction and spark plasma sintering to
improve the density and hardness of the HEBs introduced by Gild et al.
[61,333]. Their materials showed an improved relative density and high
hardness values in the range of 16.4–27.7 GPa due to the contribution of
borothermal reduction in producing high-purity and fine-grained HEBs
[331].
Qin et al. [300] synthesized five WB2- and MoB2-based HEBs by
reactive spark plasma sintering. They showed that the driving force for
the formation of these borides was quite high and their formation was
S. Akrami et al.
controlled by the kinetic issues. These HEBs, with a high relative density
and with almost no native oxides in their structure, showed a high
hardness and the highest value of 27.5 ± 1.1 GPa was achieved for
(Zr0.225Hf0.225Ta0.225Mo0.225W0.1)B2. Although WB2 and MoB2 are softer
than other binary borides in the investigated systems, their addition
even with larger grain sizes could result in a high hardness, suggesting
that the hardness of the HEBs do not follow the rule of mixtures.
Feng et al. [764] worked on (Hf,Zr,Ti,Ta,Nb)B2 and investigated the
influence of the Nb content (ranging from 0 to 20 at%) on the phase
transformation, densification, microstructure and mechanical proper­
ties. They showed that the samples have a single-phase hexagonal
structure without Nb addition and a dual-phase hexagonal structure
with different lattice parameters with Nb addition. They reported that
the relative density and grain size decrease and elastic modulus and
Vickers hardness increase to maximum values of 25.3 ± 0.6 GPa and 544
± 8 GPa, respectivel, by addition of Nb.
7.4.2. Oxidation resistance as ultrahigh-temperature ceramics
One of the first attempts to use HEBs as ultrahigh-temperature ceramics
was conducted by Gild et al. [61]. They synthesized six HEBs,
(Hf0.2Zr0.2Ta0.2Nb0.2Ti0.2)B2, (Hf0.2Zr0.2Ta0.2Mo0.2Ti0.2)B2, (Hf0.2Zr0.2Mo0.2
Nb0.2Ti0.2)B2, (Hf0.2Mo0.2Ta0.2Nb0.2Ti0.2)B2, (Mo0.2Zr0.2Ta0.2Nb0.2Ti0.2)B2
and (Hf0.2Zr0.2Ta0.2Cr0.2Ti0.2)B2, with the AlB2-type structure using ball
milling and spark plasma sintering and investigated their oxidation be­
haviors. Their results showed that all these HEBs have a better oxidation
resistance and higher hardness compared to the relevant binary borides
(except HfB2). They found that the oxidation behavior depends on not only
the compositions, but also the microstructure and synthesis route.
Tallarita et al. [324] synthesized (Hf0.2Mo0.2Zr0.2Nb0.2Ti0.2)B2 by
reactive spark plasma sintering and studied the oxidation behavior by
dynamic and isothermal thermogravimetry analysis in an air atmo­
sphere. The material showed a high oxidation resistance for tempera­
tures up to 1473 K within 6 h. The oxidation behavior of this HEB is
similar to the oxidation-resistant HfB2, but it is better than other binary
borides, such as TiB2, and TaB2, which are oxidation-resistant up to
723− 873 K.
7.4.3. Thermal conductivity for insulator coating
For ultrahigh-temperature applications, insulator coatings are
frequently used to protect various tools from thermal damage. Transi­
tion metal diborides have a high thermal conductivity due to the co-
contribution of electrons and protons, and thus, they are not consid­
ered as good thermal insulating materials [315,765–768]. Recent
studies demonstrated that the co-contribution of electrons and protons
to the thermal conductivity is weak in high-entropy materials, which
results in reducing their thermal conductivity [441,768]. Moreover,
lattice distortion and a fine grain size can more significantly reduce the
thermal conductivity of high-entropy ceramics.
The idea of a low thermal conductivity of high-entropy ceramics was
used by Chen et al. [341] to design a porous (Zr0.2Hf0.2Ti0.2Nb0.2Ta0.2)B2
for a thermal insulating application. Since the thermal conductivity
reduction is proportional to the fraction of pores (based on Kingery’s
model [769]) the key issue is uniformly increasing the fraction of pores.
They utilized borocarbothermal reduction and achieved a high fraction
of porosity of 75.67 % and small pore sizes of 0.3–1.2 μm. The thermal
diffusivity and thermal conductivity for this material were 0.74 mm2s− 1
and 0.51 Wm− 1 K− 1, respectively, which are low enough for
ultrahigh-temperature insulator coatings.
7.5. Properties of high-entropy hydrides
High-entropy hydrides are considered as a new family of materials
for hydrogen storage applications. Due to excessive consumption of
fossil fuel and global warming, hydrogen is considered as a future fuel
with zero-CO2 emissions. However, the storage of hydrogen is still a big
challenge because hydrogen gas occupies a large space and its storage
36
Materials Science & Engineering R 146 (2021) 100644
under high pressure requires special and expensive storage tanks due to
the safety requirements. The metal-to-hydride conversion systems are
the most compact and safest technology for hydrogen storage [770,771].
However, most of the metal hydrides suffer from a high thermodynamic
stability and thus they release hydrogen only after heating to high
temperatures [770,771]. Over the past decades, only limited hydrides
that can reversibly store hydrogen at room temperature were discov­
ered, such as the AB5-type LaNi5, AB2-type TiMn2 and AB-type TiFe and
BCC-based Ti-V-Cr alloys (A: elements with high chemical affinity for
hydrogen, B: elements with low chemical affinity for hydrogen)
[772–774]. However, these materials suffer either from a high cost, low
storage capacity or difficult activation (activation is usually conducted
by heating or severe mechanical treatment) [775,776]. Therefore, there
are still significant attempts to find new groups of materials for
hydrogen storage. HEAs and their HEHs are the most recent materials
that were examined for such hydrogen storage applications [777–787].
HfNbTiVZr [214], TiVZrNbHf [219], MgZrTiFe0.5Co0.5Ni0.5 [215],
Ti0.2Zr0.2Hf0.2Nb0.4 [217], Ti0.2Zr0.2Hf0.2Mo0.1Nb0.3 [217],
Ti0.2Zr0.2Hf0.2Mo0.2Nb0.2 [217], Ti0.2Zr0.2Hf0.2Mo0.3Nb0.1 [217],
Ti0.2Zr0.2Hf0.2Mo0.4 [217], TiZrNbHfTa [222,788] and MgVTiCrFe
[299] are some of the materials introduced for hydrogen absorption in
the form of HEHs. These materials usually need high temperatures over
573 K for hydrogen absorption and they produce stable HEHs which
cannot desorb hydrogen at room temperature. TiZrNbMoV [218],
TiVCrNb [223], TiVZrNb [224], TiZrHfScMo [225],
Ti0.30V0.25Zr0.10Nb0.25Ta0.10 [226] and AlCrFeMnNiW [227] are some
other HEAs which can produce HEHs, but reversible
hydriding-dehydriding of these alloys were not investigated by
pressure-composition-temperature isotherms.
Kao et al. [63] worked on CoFeMnTixVZr, CoFeMnTiVyZr and
CoFeMnTiVZrz (0.5 ≤ x ≤ 2.5, 0.4 ≤ y ≤ 3.0, and 0.4 ≤ z ≤ 3.0) with the
C14 Laves phase structure. The materials absorbed up to 1.6 wt.% of
hydrogen in the form of HEHs at room temperature, but the
pressure-composition-temperature isotherms showed that the revers­
ibility of these materials is poor at room temperature. Reversible
hydriding-dehydriding was studied at room temperature by
pressure-composition-temperature isotherms for several other HEAs
such as CoFeMnTiVZr (absorption = 1.4 wt%, desorption = 0.7 wt%)
[63], ZrTiVrCrFeNi (absorption = 1.8 wt%, desorption = 0.6 wt%)
[213], (VFe)60(TiCrCo)40-xZrx (absorption = 3.5 wt%, desorption = 2 wt
%) [220], LaNiFeVMn (absorption = 0.82 wt%, desorption = 0.2 wt%)
[221], TiZrNbTa (absorption = 1 wt%, desorption = 0.4 wt%) [789] and
TiZrNbFeNi (absorption = 1.64 wt%, desorption = 0.72 wt%) [278].
Significant amounts of hydrogen are trapped in all these HEHs and they
do not show a complete hydriding-dehydriding reversibility for
hydrogen storage.
Nygard et al. [223] suggested that the valence electron concentration
can be used as a descriptor to design materials that can reversibly store
hydrogen at room temperature. They extrapolated some experimental
data and suggested that a valence electron concentration of 6.4 is
needed to design room-temperature hydrogen storage materials. Edalati
et al. [271] and Floriana et al. [278] used this descriptor to design HEHs
for room-temperature hydrogen storage, but they added two more
criteria for such a design. (i) The C14 Laves phase is the most suitable
form of HEAs and HEHs for room-temperature hydrogen storage. (ii) The
AB2-type and AB-type alloys and their corresponding AB2H3-type and
ABH2-type hydrides are the best candidates for room-temperature
hydrogen storage. TiZrCrMnFeNi and Ti20Zr20Nb5Fe40Ni15 are two al­
loys designed based on these criteria which reversibly store up to 1.7 wt
% of hydrogen at room temperature with fast kinetics and without any
need for extra activation process. Fig. 30 shows the microstructure of
TiZrCrMnFeNi with the main C14 Laves phase structure and its
pressure-composition-temperature isotherms at room temperature for
cyclic TiZrCrMnFeNi-TiZrCrMnFeNiH6 conversion.
S. Akrami et al.
7.6. Properties of high-entropy silicides
Metal silicides are interesting materials for coatings, integrated cir­
cuit electrode films and other applications which require a high-
temperature oxidation resistivity, high electrical conductivity and
relatively high hardness [65]. Molybdenum disilicide (MoSi2) is the
most popular metal silicide which is used on an industrial scale for such
applications [790–792]. HESis were recently considered as new candi­
dates for such applications.
In 2019, Qin et al. [65] synthesized (Ti0.2Zr0.2Nb0.2Mo0.2W0.2)Si2
with the HCP structure by reactive spark plasma sintering at 1573 K.
They reported the elastic modulus and Vickers microhardness values of
352 GPa and 12.09 GPa, respectively. This hardness is higher than the
hardness of MoSi2 and is comparable to the hardness of some other
disilicides; i.e., 10.5 GPa for MoSi2 [793], 8.76 GPa for NbSi2 [794],
13.75 GPa for WSi2 [795] and 8− 10 GPa for TiSi2 [796]. Such a high
hardness level of HESi was attributed to the electronic structure,
solid-solution hardening and the Hall-Petch strengthening mechanism
[65]. They later added Al as a dopant to this HESi and could achieve the
higher hardness of 13.58 [68]. The Al dopant not only produces harder
particles but also influences the intergranular fracture and lattice slips
[797].
Gild et al. [64] introduced (Mo0.2Nb0.2Ta0.2Ti0.2W0.2)Si2 with the
C40-type hexagonal crystal structure and synthesized it by mechanical
milling and spark plasma sintering. They commented that new crystal
structures with a lower symmetry compared to binary disilicides are
achievable in HESis. They reported a Vickers hardness of 11.6 ± 0.5 GPa
which is higher than the average hardness of the corresponding binary
disilicides. Furthermore, they achieved a thermal conductivity of 6.9 ±
1.1 Wm− 1 K− 1, which is less than the average thermal conductivity of
the corresponding metal silicides [798,799]. Liu et al. [67] also syn­
thesized (Mo0.2W0.2Cr0.2Ta0.2Nb0.2)Si2 by spark plasma sintering and
investigated its mechanical properties. The elastic modulus, Vickers
micohardness and fracture toughness for this HESi were 343.8 GPa,
12.62 GPa and 2.9 MPam1/2, respectively. The hardness of this HESi is
also higher than the hardness of MoSi2.
7.7. Properties of high-entropy sulfides
Sulfides, such as Cu2SnS3, [800,801], Cu3SbS4, [802,803] and
Cu2CoSnS4 [804], are of interest because of their thermoelectric prop­
erties. Zhang et al. [69] designed two HESs, Cu5SnMgGeZnS9 and
Cu3SnMgInZnS7, by data-driven model and synthesized them by ball
milling and spark plasma sintering and studied their thermoelectric
properties. They showed that Cu3SnMgInZnS7 has a semiconducting
behavior with a high electrical resistivity and concluded that it is not a
good thermoelectric material. Cu5SnMgGeZnS9 illustrated a metallic
behavior with an electrical conductivity of 1000 Scm− 1 at 623 K, a
thermal conductivity of ~0.4 Wm− 1 K− 1 at 773 K and a Seebeck coef­
ficient of 0.6 at 873 K. These thermoelectric properties are comparable
to those reported for the ternary Cu-based and diamond-like sulfides
[805,806].
7.8. Properties of high-entropy fluorides
The optical properties of fluorides have been considered for some
applications such as laser industry [807,808], scintillators [809–811]
and ultraviolet (UV) lenses [812]. CaF2, BaF2 and SrF2 doped with rar­
e-earth ions are the most typical transparent fluorides for such appli­
cations [813–824]. There have been attempts to produce HEFs for these
optical applications [70] as well as for electrocatalytic applications [71].
Chen et al. [70] introduced a transparent HEF laser ceramic, CeN­
dCaSrBaF12, with the fluorite structure. The material was synthesized by
vacuum hot pressing which resulted in the uniform distribution of grain
sizes in the material. The material showed an in-line transmittance of
nearly 60 % at a wavelength of 1000 nm. Furthermore, there was a
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Materials Science & Engineering R 146 (2021) 100644
near-infrared photoluminescence emission band at 1057 nm and a vis­
ible-light emission band at 440 nm. These results suggest that HEFs can
be further developed to be used as a new class of transparent ceramics.
Wang et al. [71] fabricated several HEFs with the perovskite struc­
ture and used them for oxygen evolution electrocatalysis in alkaline
media. The HEFs, which were based on Na-K-Mg-Mn-Fe-Co-Ni-F
composition, were synthesized by merging a hydrothermal method
and mechanochemistry. Among all the studied HEFs, K0.8Na0.2(MgMn­
FeCoNi)F3 showed superior electrocatalytic activity for the oxygen
evolution reaction with a low overpotential of 314 mV at a current
density of 10 mAcm− 2. This overpotential is less than the one reported
for the commercial and precious IrO2, suggesting the high potential of
HEFs for electrocatalysis, Sukkurji et al. also investigated the electro­
catalytic activity of HEFs [825].
7.9. Properties of high-entropy phosphides
Metal phosphides are used as catalysts for hydrodesulfurization,
hydrogen evolution reaction, oxygen evolution reaction, Li-ion batteries
and Na-ion batteries [826]. It was shown that ternary phosphides show a
better catalytic performance in comparison to binary phosphides [827,
828]. In an attempt to produce highly-active catalysts, Zhao et al. [72]
synthesized nanosheets of an HEP containing Co, Cr, Fe, Mn and Ni using
an eutectic solvent method and examined its electrocatalytic activity for
cathodic and anodic water splitting. The HEP showed a good electro­
catalytic activity for both the oxygen and hydrogen generation with the
low cell potential of 1.78 V at the current density of 100 mAcm− 2. This
overpotential is lower than the overpotential of 1.87 V for the com­
mercial Pt/C‖IrO2 electrocatalyst at 100 mAcm− 2. The overpotential for
this HEP is lower than all binary phosphides, as shown in Fig. 31. The
higher electrocatalytic activity of this material and its lower over­
potential compared to the commercial electrocatalyst was attributed to
its structure with numerous active sites for water splitting as well as to
its high surface area in the form of nanosheets.
7.10. Properties of high-entropy phosphates
Rare-earth phosphates, such as LaPO4, with a high melting point, low
thermal conductivity and good corrosion resistance, are considered as
good environmental/thermal barrier coating materials because of their
chemical and thermal compatibility with industrial Al2O3 and ZrO2 ce­
ramics. Zhao et al. [73] synthesized a monoclinic (La0.2Ce0.2Nd0.2S­
m0.2Eu0.2)PO4 by the co-precipitation method and examined it for
environmental/thermal barrier coating applications in an Al2O3-based
composite. The HEPO4 did not react with Al2O3 at 1873 K and showed a
thermal expansion coefficient of 8.9 × 10− 6 K− 1 which is close to that of
Al2O3 and a thermal conductivity of 2.08 Wm− 1 K− 1 which is 42 % lower
than that of LaPO4. The low thermal conductivity of this material
compared to LaPO4 was attributed to its crystal structure, bonding
characteristics, phonon Umklapp scattering and lattice distortion. All
these properties make this HEPO4 a good candidate for environ­
mental/thermal barrier coatings in Al2O3-based materials. It was also
reported that HEPO4 can show good catalytic activity for oxygen evo­
lution reaction [829].
7.11. Properties of high-entropy oxynitrides
Due to recent trends in exploring oxynitride thin films for power
devices, Le et al. [74] fabricated a thin film of an oxynitride containing
Co, Cr, Fe, Mn and Ni. The material had the FCC-type structure and
produced by magnetron sputtering method followed by annealing at
1073 K. The hardness and elastic modulus of material were reported to
be 4.1 GPa and 150.5 GPa before annealing and 9.4 GPa and 156.4 GPa
after annealing, respectively. HEONs were also used as low-bandgap and
highly-stable photocatalysts for water splitting [298].
S. Akrami et al.
7.12. Properties of high-entropy carbonitrides
Cemented carbides are typical materials for cutting tools which are
normally utilized for room-temperature machining because of their su­
perior toughness and damage endurance in cyclic loadings, but their
chemical stability and oxidation resistance are not appropriate for some
severe applications [76]. Cermet materials composed of ceramics, such
as TiCN, and metal binders, such as Ni-based alloys, show a good per­
formance in the machining industries due to their good tribological
properties, high strength, good toughness and high chemical/structural
stability at high temperatures [830,831]. The concept of high-entropy
materials has been used to enhance the mechanical properties of cer­
mets for machining tools [76,832–834].
de la Obra et al. [76] introduced cermets based on HECNs and HEAs.
They used (Ti,Ta,Nb)CxN1-x as a ceramic material and CoCrFeMnNi and
CoCrFeNiV as metal binder phases. The HECNs and HEAs were first
separately synthesized by ball milling. The synthesized powders were
then mixed with a ceramic-to-metal ratio of 4/1 using milling, then
molded and finally sintered. The best mechanical properties were ach­
ieved for a composition of (Ti,Ta,Nb)CxN1-x and CoCrFeNiV which had a
hardness of 1048 Hv and a toughness of 6.8 MPam1/2. Although these
mechanical properties are weaker than the typical cermets, the idea of
high-entropy cermets seems to have a high potential for future appli­
cations in machining tools.
Recently, Dippo et al. [634,835] and Wen et al. [634,835] examined
the mechanical properties of some HECNs using the nanoindentation
technique. The measured nanohardness values, which are summarized
in Table 15, are quite high and close to 30 GPa. These hardness values
are 39 % higher than the expected hardness using the rule of mixtures
for monocarbides and mononitrides. The elastic modulus of these
HECNs are also over 500 GPa.
7.13. Properties of high-entropy borocarbonitride
In an attempt to produce ceramics with a high thermal stability,
Guana et al. [75] synthesized (Ta0.2Nb0.2Zr0.2Hf0.2W0.2)BCN,
(Ta0.2Nb0.2Zr0.2Hf0.2Ti0.2)BCN and (Ta0.2Nb0.2Zr0.2Ti0.2W0.2)BCN as
new types of ceramics. These HEBCNs were synthesized by mechanical
alloying at room temperature. Within the first 10 h of milling, the
amorphous phases were formed, but they transformed to single-phase
FCC structures by extending the milling time to 24 h. The synthesized
materials showed a uniform compositional distribution from the
micrometer scale to the nanometer scale. It was reported that these
materials remain thermally stable even after heating to 1873 K for 30
min.
7.14. Properties of high-entropy ceramic-ceramic composites
There have been limited attempts to produce high-entropy ceramic-
ceramic composites for possible applications at low [836] and high
temperatures [837]. Qin et al. [837] mixed hexagonal
Ti-Zr-Nb-Hf-Ta-W-based HEBs with cubic Ti-Zr-Nb-Hf-Ta-W-based HECs
by ball-milling followed by spark plasma sintering. They added 24, 45,
65 and 83 wt% HECs to HEBs and compared the resultant grain size,
hardness and thermal conductivity of the composites to those of
(Ti0.22Zr0.19Nb0.18Hf0.19Ta0.19W0.03)B2 and (Ti0.20Zr0.21Nb0.21Hf0.18­
Ta0.17W0.03)C. They showed that the grain size and mechanical prop­
erties can be tuned by changing the fraction of each phase: increasing
the fraction of the HECs in the composites resulting in larger grain sizes,
higher hardness, lower elastic modulus and lower thermal conductivity.
They also reported that the hardness levels of the composites were better
than the values calculated by the rule of mixtures.
8. Concluding remarks and outlook
The concept of entropy stabilization by increasing the number of
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Materials Science & Engineering R 146 (2021) 100644
principal elements to five or more has been resulted in the introduction
of various high-entropy alloys and ceramics. Despite the significant
studies of high-entropy alloys, research activities regarding high-
entropy ceramics have been enhanced only in recent years. There is
now a wide range of high-entropy ceramics including oxides, nitrides,
carbides, borides, hydrides, silicides, sulfides, fluorides phosphides,
phosphates, oxynitrides, carbonitrides and borocarbonitrides. High-
entropy nitrides are the first kind of high-entropy ceramics which
were introduced in 2004, but high-entropy oxides and carbides are the
most investigated ones. The current review paper covers the majority of
publications from November 2004 to August 2021 and discusses the
principles (Section 2), history (Section 3), crystal structure (Section 4),
theoretical/empirical design (Section 5), production methods (Section
6), properties and potential applications (Section 7) of this new family of
materials.
High-entropy ceramics with a configuration entropy higher than
1.5R (R: gas constant) contain five or more cations in their structure.
Their main crystal structures include rock-salt, fluorite, perovskite,
pyrochlore and spinel, although many other structures have been re­
ported for these ceramics. There have been successful attempts to design
these materials by theoretical computation using density functional
theory, molecular dynamics simulation, conventional thermodynamic
calculation, CALPHAD method, machine learning and neural network.
Moreover, for the design of these materials, there have been some suc­
cesses when using empirical methods and descriptors such as the
entropy-forming ability, Goldschmid tolerance factor, size disorder
factor and valence electron concentration. For the synthesis of high
entropy ceramics, there have been significant attempts to use various
conventional methods including solid-state synthesis, liquid-state syn­
thesis and gas-state synthesis, as discussed in Section 6. These methods
can be effectively used to fabricate powders, bulk samples, thin films,
nanosheets, nanotubes, etc. The properties of high-entropy ceramics
have been investigated for different potential applications, as discussed
in Section 7. Their properties include mechanical properties, thermal
properties, catalytic properties, ionic conductivity, electrical properties,
magnetic properties, optical properties, biocompatibility, oxidation
resistance, corrosion resistance and hydrogen storage performance.
Such a wide range of properties, which are very often superior compared
to conventional ceramics, indicate the high potential of this new family
of materials for future applications and commercialization.
Since high-entropy ceramics with various crystal structures can be
formed by selection of a wide range of different atoms, it is possible to
achieve promising properties for different applications by adjusting the
composition and structure of these ceramics. Since the nature of atoms
and their location in crystal structure determine the final properties, a
combination of materials science, theoretical computation and synthesis
methods can facilitate the development of these functional materials for
future applications. While the design of advanced high-entropy ceramics
is still the main scientific challenge, development of synthesis methods
at the industrial scale will be a task for commercialization of these
materials in the future. By considering the high demands in realizing the
carbon-neutral energy to reduce the CO2 emission and by considering
the promising energy-related properties reported so far for the high-
entropy ceramics, it is expected that these materials will contribute to
the energy issues in the future.
Declaration of Competing Interest
The authors declare that they have no known competing financial
interests or personal relationships that could have appeared to influence
the work reported in this paper.
Acknowledgments
The author KE acknowledges the MEXT, Japan for Grants-in-Aid for
Scientific Research on Innovative Areas (No. 19H05176 and No.
S. Akrami et al. Materials Science & Engineering R 146 (2021) 100644

21H00150).

Appendix A

A summary of the studies published from November 2, 2004 to

February 20, 2021 are presented in Tables A1–A6 for the HEOs, HENs,
HECs, HEBs, HEHs and other high entropy ceramics, respectively.
Tables A1–A6 cover the material composition, sample shape, crystal
structure, synthesis method and investigated properties.

Table A1
Summary of publications about high-entropy oxides in chronological order.
Ceramic Composition Sample Crystal Structure Synthesis Method Investigated Properties Reference
Shape

AlxCoCrCuFeNi-O (x = 0.5, 1, 2) Film Spinel Sputtering Hardness and bandgap Chen et al.
deposition (2007) [56]
Spinel: Sputtering Mechanical and thermal Chen et al.
Cubic (773 K) deposition properties (2008) [57]
AlxCoCrCuFeNi-O Film Tetragonal (973 K)
Orthorhombic
(1173 K)
Lin et al. (2009)
(Bi1-x-yNa0.925-x-yLi0.075)0.5BaxSryTiO3 Disk Perovskite Ball mill & sintering Electrical properties
[302]
Magnetron Mechanical, electrical and Lin et al. (2010)
(AlCrTaTiZr)Ox Film Amorphous
sputtering optical properties [201]
TixFeCoNi-O (x = 0, 0.25, 0.5, 0.75, 1) TiFeCoNiCux-O (x = 1, 2,
DC physical vapor Tsau et al.
3) Film FCC Electrical resistivity
sputtering (2012) [208]
AlxCrFeCoNiCu-O (x = 0.5, 1)
0.4541Pb(Mg1/3Nb2/3)⋅0.0982Pb(Zn1/3Nb2/3).0.1477Pb(Ni1/ Talanov (2013)
Disk Perovskite Solid-state sintering Dielectric properties
3Nb2/3)⋅0.3PbTiO3 [400]
CrFeCoNiOx
Arc melting and Tsau et al.
AlFeCoNiOx Film Amorphous Electrical resistivity
annealing (2015). [560]
TiFeCoNiOx
Rock-salt +
Tenorite (> 973 K) Solid-state reaction Rost et al.
MgO-CoO-NiO-CuO-ZnO Pellet Phase transformation
Rock-salt (> 1123 & pressing (2015) [58]
K)
Dielectric and Zachariasz et al.
Pb0.94Sr0.06(Zr0.50Ti0.50)0.99Cr0.01O3 Pellet Perovskite Ball mill & sintering
piezoelectric properties (2015) [148]
D. Berardan
(MgCoNiCuZn)1-x-yGayAxO (with A = Li, Na, K) Pellet Rock-salt Ball mill & pressing Li ion conductivity
(2016) [113]
I. (Mg0.1Co0.1Ni0.1Cu0.1Zn0.1)O0.5 I. Pellet Rock-salt I. Ball mill Synthesis and electronic
Rak et al. (2016)
II. (Mg0.1Co0.1Ni0.1Cu0.1Zn0.1)O0.5 + Li II. Film II. Pulsed laser states by experiments and
[87]
III. (Mg0.1Co0.1Ni0.1Cu0.1Zn0.1)O0.5 + Sc III. Film deposition DFT calculations
Optimizing synthesis Cestari et al.
Si-Al-P-Ca-F-O Powder Amorphous Sol-gel
process (2016) [203]
Thermal analysis and Shankhwar et al.
43SiO2⋅24.5CaO⋅24.5Na2O⋅6P2O5⋅2Fe2O3 Powder Amorphous Modified sol–gel
magnetic properties (2016) [202]
(Mg,Co,Ni,Cu,Zn)1-xLixO
Bérardan et al.
(Mg,Co,Ni,Cu,Zn)1− 2x(LiGa)xO Pellet Rock-salt Ball mill & sintering Dielectric constant
(2016) [88]
(Mg,Co,Ni,Cu)0.8(LiGa)0.2O
Optimizing synthesis
Berardan et al.
(Mg,Co,Cu,Ni,Zn)O Bar Rock-salt Ball mill & sintering process and crystal
(2017) [89]
structure
Rost et al.
Mg0.2Ni0.2Co0.2Cu0.2Zn0.2O Powder Rock-salt Ball mill Local atomic structure
(2017) [90]
Meisenheimer
Pulsed laser
(Mg0.25(1-x)CoxNi0.25(1-x) Cu0.25(1-x)Zn0.25(1-x))O Film Cubic Magnetic properties et al. (2017)
deposition
[389]
(Co,Mg,Ni,Zn)O Nebulized spray
pyrolysis, flame
Crystal structure and Sarkar et al.
Powder Rock-salt spray pyrolysis &
(Co,Cu,Mg,Ni,Zn)O phase compositions (2017) [103]
reverse co-
precipitation
(Ce,La,Pr)O
(Ce,La,Pr,Y)O
(Ce,La,Pr,Sm)O Nebulized spray Djenadic et al.
Powder CaF2-type Crystal structure
(Ce,La,Pr,Sm,Y)O pyrolysis (2017) [127]
(Ce,La,Nd,Pr,Sm,Y)O
(Ce,Gd,La,Nd,Pr,Sm,Y)O
Nebulized spray Sarkar et al.
(Ce/Gd/La/Nd/Pr/Sm/Y)-O Powder Fluorite Bandgap
pyrolysis (2017) [128]
Chen et al.
(Ce0.2Zr0.2Hf0.2Sn0.2Ti0.2)O2 Disk Fluorite Ball mill & sintering Thermal conductivity
(2018) [448]
(continued on next page)

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S. Akrami et al. Materials Science & Engineering R 146 (2021) 100644

Table A1 (continued )
Ceramic Composition Sample Crystal Structure Synthesis Method Investigated Properties Reference
Shape

(Gd0.2La0.2Nd0.2Sm0.2Y0.2)CoO3
(Gd0.2La0.2Nd0.2Sm0.2Y0.2)CrO3
(Gd0.2La0.2Nd0.2Sm0.2Y0.2)FeO3
(Gd0.2La0.2Nd0.2Sm0.2Y0.2)MnO3
(Gd0.2La0.2Nd0.2Sm0.2Y0.2)NiO3
Nebulized spray Microstructure and crystal Sarkar et al.
Gd(Co0.2Cr0.2Fe0.2Mn0.2Ni0.2)O3 Powder Perovskite
pyrolysis structure (2018) [136]
La(Co0.2Cr0.2Fe0.2Mn0.2Ni0.2)O3
Nd(Co0.2Cr0.2Fe0.2Mn0.2Ni0.2)O3
Sm(Co0.2Cr0.2Fe0.2Mn0.2Ni0.2)O3
Y(Co0.2Cr0.2Fe0.2Mn0.2Ni0.2)O3
(Gd0.2La0.2Nd0.2Sm0.2Y0.2)(Co0.2Cr0.2Fe0.2Mn0.2Ni0.2)O3
(Hf0.25Zr0.25Ce0.25Y0.25)O2-δ
(Hf0.25Zr0.25Ce0.25) (Y0.125Yb0.125)O2-δ
(Hf0.2Zr0.2Ce0.2)(Y0.2Yb0.2)O2-δ
(Hf0.25Zr0.25Ce0.25)(Y0.125Ca0.125)O2-δ Ball mill & spark Thermal and electrical Gild et al.
Disk Fluorite
(Hf0.25Zr0.25Ce0.25) (Y0.125Gd0.125)O2-δ plasma sintering conductivity and hardness (2018) [118]
(Hf0.2Zr0.2Ce0.2)(Y0.2Gd0.2)O2-δ
(Hf0.25Zr0.25Ce0.25)(Yb0.125Gd0.125)O2-δ
(Hf0.2Zr0.2Ce0.2) (Yb0.2Gd0.2)O2-δ
Ag14.3V14.3Te9.5O61.9
Pb9.7Ti1.7Te16.9B10O61.7
Mo11.4W2.9Te14.3O71.4
Bi11.1Mo10.3Te10.3O68.3
Cu7.3Na17.1P17.1O58.5
Bi14.3Ti2.4Te7.1B14.3O61.9
Ga9.7Zn4.9P18.9O66.5
Cassar et al.
Ba4.7Cu0.3K5.2Zn3.1B30.5O56.2 Predicting glass transition temperatures using neural networks
(2018) [257]
Cu12.8Ti3.8P17.9O65.5
Ca2.9Fe2.1Mg4.2Na0.4P16.8B8.4O65.2
Ca5.1Fe0.1K8.1Mg3.9Mn0.3Na1.2All0.4P1.4Si19.8O59.7
Ca15.8Na2.6Nb2.6P15.8O63.2
Li1.9Mg0.3Zn0.4Zr0.5Ti0.5Al10.2P3.7B2.7Si15.8O64
Ca1.9Mg2.5Sr1.9Al6.9B5Si19.2O62.6
La7.3Al16.6P6.7Si5.7O63.7
Rák et al. (2018)
(MgCoNiZn)1-xCuxO (x = 0.13, 0.2, 0,.26) Local atomic configuration by DFT calculations
[240]
Sr(Zr0.2Sn0.2Ti0.2Hf0.2Mn0.2)O3
Sr(Zr0.2Sn0.2Ti0.2Hf0.2Nb0.2)O3
Ba(Zr0.2Sn0.2Ti0.2Hf0.2Ce0.2)O3 Jiang et al.
Pellet Perovskite Ball mill & sintering Crystal structure
Ba(Zr0.2Sn0.2Ti0.2Hf0.2Y0.2)O3 (2018) [139]
Ba(Zr0.2Sn0.2Ti0.2Hf0.2Nb0.2)O3
(Sr0.5Ba0.5)(Zr0.2Sn0.2Ti0.2Hf0.2Nb0.2)O3
Co-precipitation &
Biesuz et al.
(Mg,Co,Ni,Cu,Zn)O Powder Rock-salt hydrothermal Thermal evolution
(2018) [109]
synthesis
(Co0.2Cu0.2Mg0.2Ni0.2Zn0.2)O TM-HEO
(Co0.25Cu0.25Mg0.25Ni0.25)O TM-MEO(-Zn) Nebulized spray Sarkar et al.
Powder Rock-salt Li conductivity
(Co0.25Mg0.25Ni0.25Zn0.25)O TM-MEO(-Cu) pyrolysis (2018) [104]
(Cu0.25Mg0.25Ni0.25Zn0.25)O TM-MEO(-Co)
(Mg,Co,Cu,Ni,Zn)O
(Ca,Co,Cu,Ni,Zn)O
(Mg,Co,Cu,Ni)O
Anand et al.
(Mg,Co,Cu,Zn)O Configurational entropy calculation by classic thermodynamic simulations
(2018) [256]
(Mg,Co,Ni,Zn)O
(Mg,Cu,Ni,Zn)O
(Co,Cu,Ni,Zn)O
Ball mill & spark Performance under Gwalani et al.
Al0.3CoCrFeMnNi + 3 vol% Y2O3 Pellet FCC
plasma sintering mechanical loading (2018) [209]
Pulsed laser Thermal stability and Kotsonis et al.
MgxNixCoxCuxZnxScxO (x = 0.167) Film Rock-salt
deposition phase transformation (2018) [445]
Pulsed Crystal structure and Sharma et al.
Ba(Zr0.2Sn0.2Ti0.2Hf0.2Nb0.2)O3 Film Perovskite
laser deposition growth orientation of film (2018) [140]
MgxNixCuxCoxZnxO, x = 0.2
MgxNixCuxCoxZnxScxO, x = 0.167
MgxNixCuxCoxZnxSbxO, x = 0.167 Pulsed laser Thermal and mechanical Braun et al.
Film Rock-salt
MgxNixCuxCoxZnxSnxO, x = 0.167 deposition properties (2018) [441]
MgxNixCuxCoxZnxCrxO, x = 0.167
MgxNixCuxCoxZnxGexO, x = 0.167
Bulk: Press &
(Mg0.25(1-x)CoxNi0.25(1-x)Cu0.25(1-x)Zn0.25(1-x))O
sintering Chemical homogeneity, Sivakumar et al.
Bulk & Film Rock-salt
Film: Laser surface topography (2018) [115]
(Mg0.25(1-x)Co0.25(1-x)Ni0.25(1-x)CuxZn0.25(1-x))O
deposition
Arc melting & Lei et al. (2018)
TaNbHfZrTi-O Nanotube Amorphous
anodic oxidation [204]
(continued on next page)

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Table A1 (continued )
Ceramic Composition Sample Crystal Structure Synthesis Method Investigated Properties Reference
Shape

Morphology,
microstructure and
thermal stability
(Co,Cr,Fe,Mn,Ni)3O4 Pellet Spinel Vibrational mill & Microstructure Dąbrowa et al.
sintering (2018) [164]
(Co,Cu,Mg,Ni,Zn)O Pellet Rock-salt Ball mill & sintering Phase stability Dupuy et al.
(2019) [93]
(Na0.2Bi0.2Ba0.2Sr0.2Ca0.2)TiO3 Disk Perovskite Ball mill & sintering Dielectric properties Pu et al. (2019)
[149]
(CuNiFeCoMg)Ox-Al2O3 Powder Cubic Nonhydrolytic sol- Catalysis Zhang et al.
gel (2019) [349]
Mg0.2Co0.2Ni0.2Cu0.2Zn0.2O Powder FCC Bal mill & sintering Li ion conductivity Qiu et al. (2019)
& ball mill [210]
(MgCoNiCuZn)O Pellet Rock-salt Ball mill & pressing Li conductivity Osenciat et al.
(2019) [92]
CrFeCoNiMn-O Disk Cubic Arc melting & Physicomechanical Ghorban et al.
deposition performance (2019) [443]
Mg0.2Co0.2Ni0.2Cu0.2Zn0.2O Pellet Rock-salt Solid-state reaction Magnetic properties Jimenez-Segura
& pressing et al. (2019)
[98]
(Co0.2Cu0.2Mg0.2Ni0.2Zn0.2)O Powder Rock-salt Solution combustion Magnetic properties Mao et al.
(2019) [110]
10La2O3-20TiO2-10Nb2O5-20WO3-20ZrO2 Spheres Amorphous Containerless Glass transition Zhang et al.
solidification via temperature, hardness (2019) [206]
aerodynamic and optical bandgap
levitation
(Al0.31Cr0.20Fe0.14Ni0.35)O Film Rock-salt Magnetron Mechanical properties Yang et al.
sputtering (2019) [444]
Rock-salt +
Tenorite (1.5 h
Catalyst activity for CO2 Chen et al.
(NiMgCuZnCo)O Powder milling) Ball mill
to CO conversion (2019) [94]
Rock-salt (2 h
milling)
I. (Co0.2Cu0.2Mg0.2Ni0.2Zn0.2)O Nebulized spray Li ion conductivity: I) Wang et al.
Powder Rock-salt
II. LiNi1/3Co1/3Mn1/3O2 pyrolysis anode and II) cathode (2019) [101]
I. (Co0.2Cu0.2Mg0.2Ni0.2Zn0.2)O Powder I. Rock-salt Nebulized spray
Microstructure and Chellali et al.
II. (Ce0.2La0.2Pr0.2Sm0.2Y0.2)O2-δ II. Fluorite pyrolysis & high-
Pellet structural composition (2019) [102]
III.(Gd0.2La0.2Nd0.2Sm0.2Y0.2)(CO0.2Cr0.2Mn0.2Fe0.2Ni0.2)O3 III. Perovskite pressure torsion
Precipitation & Phase composition and Sachkov et al.
(Sc0.2Ce0.2Pr0.2Gd0.2Ho0.2)2O3±δ Powder Fluorite
annealing structure (2019) [121]
Zhang et al.
(Mg0.2Co0.2Ni0.2Cu0.2Zn0.2)O Powder Rock-salt Solid-state reaction Magnetic structure
(2019) [77]
Magnetron Kirnbauer et al.
(Al0.19Cr0.13Nb0.19Ta0.30Ti0.19)O2 Film Rutile-type Mechanical properties
sputtering (2019) [196]
Powder Balcerzak et al.
(Co,Cu,Mg,Ni,Zn)O Rock-salt Ball mill & sintering Electrical properties
Bulk (2019) [95]
Bochenek et al.
Pb(Zr0.49Ti0.51)0.94Mn0.014Sb0.02W0.014Ni0.02O3 Bulk Perovskite Ball mill & sintering Electrophysical behavior
(2019) [150]
Hanioka et al.
Y1–x–yErxYbyBaZn3AlO7 Powder Hexagonal Flux method Wavelength conversion
(2019) [574]
Solvothermal Electrocatalysis for water Wang et al.
(Co,Cu,Fe,Mn,Ni)3O4 Powder Spinel
method oxidation (2019) [82]
Li et al. (2019)
(Li0.06Na0.47K0.47)(Nb0.94Sb0.06)O3 Powder Perovskites Molten salt method Piezoelectric properties
[143]
Dielectric,
electromagnetic
Co-precipitation & Radoń et al.
(Zn,Mg,Ni,Fe,Cd)Fe2O4 Powder Spinel interference shielding and
annealing (2019) [205]
microwave absorption
properties
Spinel + FCC + Sol–gel auto- Lal et al. (2019)
Ni-Fe-Co-Cr-Al-O Powder Catalysis
BCC combustion [162]
Nebulized spray Pressure effect on Cheng et al.
(Ce0.2La0.2Pr0.2Sm0.2Y0.2)O2− Powder CaF2-type
pyrolysis structure and bandgap (2019) [211]
δ

Modified solution Optimizing synthesis and Mao et al.

(CoCrFeMnNi)3O4 Powder Spinel
combustion magnetic properties (2019) [159]
Reactive spark Biesuz et al.
Sr((Zr0.94Y0.06)0.2Sn0.2Ti0.2Hf0.2Mn0.2)O3− x Bar Perovskite Crystal structure
plasma sintering (2019) [142]
Zheng et al.
Ni-Mg-Cu-Zn-Co-O Powder Rock-salt Ball mill Catalysis for Li-S batteries
(2019) [97]
Gd(Co0.2Cr0.2Fe0.2Mn0.2Ni0.2)O3
La(Co0.2Cr0.2Fe0.2Mn0.2Ni0.2)O3
Magnetic properties and
Nd(Co0.2Cr0.2Fe0.2Mn0.2Ni0.2)O3 Nebulized spray Witte et al.
Powder Perovskite Mössbauer
Sm(Co0.2Cr0.2Fe0.2Mn0.2Ni0.2)O3 pyrolysis (2019) [79]
characterization
Y(Co0.2Cr0.2Fe0.2Mn0.2Ni0.2)O3
(Gd0.2La0.2Nd0.2Sm0.2Y0.2)(Co0.2Cr0.2Fe0.2Mn0.2Ni0.2)O3
(continued on next page)

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Table A1 (continued )
Ceramic Composition Sample Crystal Structure Synthesis Method Investigated Properties Reference
Shape

(La0.2Ce0.2Nd0.2Sm0.2Eu0.2)2Zr2O7 Powder Pyrochlore Co-precipitation Thermal conductivity Zhao et al.

(2019) [176]
(Yb0.2Y0.2Lu0.2Sc0.2Gd0.2)2Si2O7 Powder Monoclinic Sol-gel Environmental coating for Dong et al.
SiC-based composites (2019) [197]
(La0.2Nd0.2Sm0.2Eu0.2Gd0.2)2Zr2O7
(Y0.2Nd0.2Sm0.2Eu0.2Gd0.2)2Zr2O7 Pellet
Microstructures and
(La0.2Y0.2Sm0.2Eu0.2Gd0.2)2Zr2O7 Li et al. (2019)
Pyrochlore Ball mill & sintering thermal conductivity for
(La0.2Nd0.2Y0.2Eu0.2Gd0.2)2Zr2O7 [83]
thermal barrier coating
(La0.2Nd0.2Sm0.2Y0.2Gd0.2)2Zr2O7
(La0.2Nd0.2Sm0.2Eu0.2Y0.2)2Zr2O7
Mechanical and thermal
Ball mill & hot Ren et al. (2019)
(Y1/4Ho1/4Er1/4Yb1/4)2SiO5 Bulk Monoclinic properties as thermal
pressing [198]
barrier coating
Effect of mass and charge disorder on phonon thermal conductivity by molecular dynamics Lim et al. (2019)
(Mg0.1Co0.1Ni0.1Cu0.1Zn0.1)O0.5 + Sc, Sn, Cr, Ge
simulations [401]
Grzesik et al.
(Co,Cu,Mg,Ni,Zn)O Pellet Rock-salt Ball mill & sintering Defect structure
(2019) [99]
Hong et al.
(Mg,Co,Ni,Cu,Zn)O Pellet Rock-salt Ball mill & Sintering Mechanical properties
(2019) [100]
Musicó et al.
(Mg/Cr/Mn/Co/Fe/Ni/Cu/Zn)(Cr/Fe/Al)2O4 Cubic Fm-3 m Solid-state reaction Magnetic properties
(2019) [402]
Sarkar et al.
HEOs Review on electrochemical properties
(2019) [32]
I. BaO-SrO-CaO-La2O3-Fe2O3-Al2O3-TiO2-Cr2O3-Ga2O3-In2O3- I.
CuO Magnetoplumbite Vinnik et al.
Pellet Ball mill & sintering Magnetic properties
II. BaO-SrO-CaO-La2O3-Fe2O3-Al2O3-Cr2O3-CoO-Ga2O3-In2O3- II. Spinel + (2020) [200]
WO3 Tungstate
BaO-SrO-CaO-MgO-PbO-TiO2
Vinnik et al.
BaO-SrO-CaO-MgO-PbO-Fe2O3 Pellet Perovskite Solid-state sintering Dielectric properties
(2020) [141]
Na2O-K2O-CaO-La2O3-Ce2O3-TiO2
Chen et al.
(Mg0.2Ti0.2Zn0.2Cu0.2Fe0.2)3O4 Pellet Spinel Ball mill & Sintering Li ion conductivity
(2020) [156]
Amorphous (873 Polymeric steric
Tseng et al.
Gd0.4Tb0.4Dy0.4Ho0.4Er0.4O3 Pellet K) entrapment method Phase transformation
(2020) [195]
Bixbyite (1299 K) & sintering
(Gd0.2La0.2Nd0.2Sm0.2Y0.2)CoO3
Nebulized spray Witte et al.
(Gd0.2La0.2Nd0.2Sm0.2Y0.2)FeO3 Powder Perovskite Magnetic properties
pyrolysis (2020) [137]
(Gd0.2La0.2Nd0.2Sm0.2Y0.2)CrO3
(Co,Cr,Fe,Mn,Ni)3O4
Thermal and electrical Stygar et al.
(Co,Cr,Fe,Mg,Mn)3O4 Pellet Spinel Ball mill & sintering
properties (2020) [157]
(Cr,Fe,Mg,Mn,Ni)3O4
Flash-assisted Kumar et al.
(Mg,Co,Cu,Ni,Zn)O Pellet Rock-salt Crystal structure
synthesis (2020) [106]
Reaction-assisted Liu et al. (2020)
(Mg0.2Ni0.2Co0.2Cu0.2Zn0.2)O Pellet Rock-salt Phase transition
flash sintering [107]
Phase stability, anisotropy Chen et al.
(Yb0.25Y0.25Lu0.25Er0.25)2SiO5 Powder Monoclinic Solid-state reaction
and thermal expansion (2020) [199]
Crystal structure and Grzesik et al.
(Co,Cr,Fe,Mn,Ni)3O4 Pellet Spinel Ball mill & sintering
thermal stability (2020) [158]
Facile solution Mao et al.
(Al1/6Co1/6Cr1/6Fe1/6Mn1/6Ni1/6)3O4 Powder Spinel Magnetic property
combustion (2020) [160]
Gd2Zr2O7
(Gd1/2Eu1/2)2Zr2O7
(Gd1/3Eu1/3Sm1/3)2Zr2O7
Teng et al.
(Gd1/4Eu1/4Sm1/4Nd1/4)2Zr2O7 Pellet Pyrochlore Ball mill & sintering Structural investigation
(2020) [174]
(Gd1/5Eu1/5Sm1/5Nd1/5La1/5)2Zr2O7
(Gd1/6Eu1/6Sm1/6Nd1/6La1/6Dy1/6)2Zr2O7
(Gd1/7Eu1/7Sm1/7Nd1/7La1/7Dy1/7Ho1/7)2Zr2O7
NiFe1.9(Dy0.02Er0.02Gd0.02Ho0.02Tb0.02)O4
(Co0.2Cr0.2Fe0.2Mn0.2Ni0.2)Fe2O4 Sol-gel auto- Effect of entropy on Parida et al.
Powder Spinel
(Co0.2Cr0.2Fe0.2Mn0.2Ni0.2)Fe1.9(Dy0.02Er0.02Gd0.02Ho0.02Tb0.02) combustion stability (2020) [163]
O4
Yoon et al.
Mg0.2Ni0.2Co0.2Cu0.2Zn0.2O Powder Rock-salt Polymeric synthesis Optimizing synthesis
(2020) [108]
Spiridigliozzi
Hydrothermal
Ce0.2Zr0.2Y0.2Gd0.2La0.2O2− d Powder Fluorite Thermal behavior et al. (2020)
method
[120]
Pb0.95Ba0.05(Mg1/3Nb2/3)0.471(Zn1/3Nb2/3)0.102 (Ni1/3Nb2/ Solid-state reaction Electromechanical Talanov et al.
Disk Rhombohedral
3)0.152Ti0.275O3 & sintering properties (2020) [403]
Fluorite + Combustion & ball Phase composition and Zhang et al.
(La0.2Nd0.2Sm0.2Gd0.2Yb0.2)2Zr2O7 Nanopowder
Pyrochlore mill & sintering crystal structure (2020) [404]
Co- precipitation &
Mechanical and thermal Ren et al. (2020)
((Sm0.2Eu0.2Tb0.2Dy0.2Lu0.2)2Zr2O7 Bulk Pyrochlore spark plasma
properties [177]
sintering
BaSr(ZrHfTi)O3 Perovskite Catalysis
(continued on next page)

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Table A1 (continued )
Ceramic Composition Sample Crystal Structure Synthesis Method Investigated Properties Reference
Shape

BaSrBi(ZrHfTiFe)O3 Nano- Sonochemical-based Okejiri et al.

Ru/BaSrBi(ZrHfTiFe)O3 particles method (2020) [80]
Dielectric, piezoelectric Pavelko et al.
xPbTiO3-yPbZrO3-zPbNb2/3Mg1/3O3 Powder Perovskite Solid-state reaction
and elastic properties (2020) [405]
La2Zr2O7
Sm2Zr2O 7
La2(Hf1/2Zr1/2)2O7
Sm2(Sn1/4Ti1/4Hf1/4Zr1/4)2O7
Gd2(Sn1/4Ti1/4Hf1/4Zr1/4)2O7
(Sm1/2Gd1/2)2(Ti1/3Hf1/3Zr1/3)2O7
(Eu 1/2Gd1/2)2(Ti1/3Hf1/3Zr1/3)2O7
(La1/2Pr1/2)2(Sn1/3Hf1/3Zr1/3)2O7
(Eu1/2Gd1/2)2(Sn1/3Hf1/3Zr1/3)2O7
(La1/3Pr1/3Nd1/3)2(Hf1/2Zr1/2)2O7
(Sm1/3Eu1/3Gd1/3)2(Hf1/2Zr1/2)2O7 Mechanical and thermal Wright et al.
Pellet Pyrochlores Ball mill & sintering
(Sm1/3Eu1/3Gd1/3)2(Sn1/3 Hf1/3Zr1/3)2O7 properties (2020) [175]
(Sm1/3Eu1/3Gd1/3)2(Ti1/4Sn1/4Hf1/4Zr1/4)2O7
(Sm1/4Eu1/4Gd1/4Yb1/4)2(Ti1/4Sn1/4Hf1/4Zr1/4)2O7
(Sm1/3Eu1/3Gd1/3)2(Ti1/2Sn1/6Hf1/6Zr1/6)2O7
(Sm1/3Eu1/3Gd1/3)2(Ti3/4Sn1/12Hf1/12Zr1/12)2O7
(Sm1/3Eu1/3Gd1/3)2Ti2O7
(Sm1/4Eu1/4Gd1/4Yb1/4)2(Ti1/2Hf1/4Zr1/4)2O7
(Sm3/4Yb1/4)2(Ti1/2Zr1/2)2O7
(La1/5Ce1/5Nd1/5Sm1/5Eu1/5)2Zr2O7
(La1/7Ce1/7Pr1/7Nd1/7Sm1/7Eu1/7Gd1/7)2(Hf1/2Zr1/2)2O7
(La1/7Ce1/7Pr1/7Nd1/7Sm1/7Eu1/7Gd1/7)2(Sn1/3Hf1/3Zr1/3)2O7
I. (Tm0.2Y0.2Pr0.2Gd0.2Dy0.2)3Si2C2/
(Tm0.2Y0.2Pr0.2Gd0.2Dy0.2)2O3) Electromagnetic Chen et al.
Powder Orthorhombic Ball mill
II. (Tm0.2Y0.2Pr0.2Gd0.2Tb0.2)3Si2C2/ absorption capability (2020) [406]
(Tm0.2Y0.2Pr0.2Gd0.2Tb0.2)2O3)
1.(MgZnMnCoNi)Ox Nguyen et al.
Film Spinel + Rock-salt Sputtering Structural features
2.(CrFeMnCoNi)Ox (2020) [386]
Application in Li-ion Wang et al.
(FeCoNiCrMn)3O4 Powder Spinel Solid-state reaction
battery (2020) [525]
Application in Li-ion Tavani et al.
(Mg0.2Co0.2Ni0.2Cu0.2Zn0.2)O Powder Rock-salt Solid-state reaction
battery (2020) [526]
(Ce,Gd,Nd,Sm,Pr)O2-δ Crystal and structure and Dąbrowa et al.
Pellet Fluorite Ball mill & sintering
(Ce,Gd,La,Nd,Pr)O2-δ electrical properties (2020) [119]
Application in Li-ion Ghigna et al.
(Mg0.2Co0.2Ni0.2Cu0.2Zn0.2)O Powder Rock-salt Solid-state reaction
battery (2020) [114]
Chen et al.
(NiMgCuZnCo)O Powder Rock-salt Ball mill Catalysis
(2020) [467]
Flame spray
pyrolysis, nebulized
Usharani et al.
(Co,Cu,Mg,Ni,Zn)O Powder Rock-salt spray pyrolysis & Magnetic properties
(2020) [105]
reverse co-
precipitation
Ball mill & spark Zhao et al.
(Y0.25Yb0.25Er0.25Lu0.25)2(Zr0.5Hf0.5)2O7 Bulk Fluorite Thermal properties
plasma sintering (2020) [78]
(Hf1/3Zr1/3Ce1/3)1-x(Y1/2X1/2)xO2-δ Mechanical and thermal Wright et al.
Pellet Fluorite Ball mill & sintering
(X = Yb, Ca, Gd; x = 0.4, 0.148, 0.058) properties (2020) [39]
Al97Fe0.5Ni1.5-O
Fang et al.
Al97.5Fe0.5Co0.5Ni1.5-O Ribbon FCC Dealloying Catalysis
(2020) [374]
Al97Fe0.5Co0.5Ni1.5X0.5-O (X: Mo, V, Cr, Nb, Ti, Cu, Mn)
I. Ba(Zr0.2Ti0.2Sn0.2Hf0.2V0.2)O3 I-III. multi-phases
II. Ba(Zr0.2Ti0.2Sn0.2Hf0.2Mo0.2)O3
III. Ba(Zr0.2Ti0.2Sn0.2Hf0.2W0.2)O3 Zhou et al.
Pellet Ball mill & sintering Dielectric properties
IV. Ba(Zr0.2Ti0.2Sn0.2Hf0.2Y0.2)O3 IV-VI. Perovskite (2020) [151]
V. Ba(Zr0.2Ti0.2Sn0.2Hf0.2Nb0.2)O3
VI. Ba(Zr0.2Ti0.2Sn0.2Hf0.2Ta0.2)O3
Wang et al.
Sr(Ti0.2Y0.2Zr0.2Sn0.2Hf0.2)O3-x Bulk Perovskite Flash sintering Optimizing synthesis
(2020) [144]
Pulsed laser Patel et al.
(La0.2Pr0.2Nd0.2Sm0.2Eu0.2)NiO3 Film Perovskite Electronic behavior
deposition (2020) [146]
Yan et al. (2020)
[(Bi,Na)1/5(La,Li)1/5(Ce,K)1/ 5Ca1/5Sr1/5]TiO3 Pellet Perovskite Ball mill & sintering Li ion conductivity
[153]
(Cr0.2Fe0.2Mn0.2Ni0.2Zn0.2)3O4 Mao et al.
Powder Spinel Solution combustion Magnetic properties
(Cr0.2Fe0.2Mn0.2Co0.2Zn0.2)3O4 (2020) [161]
Melt spinning & Ding et al.
Fe-Co-Ni-Cr-Nb-O Film Amorphous Catalysis
dealloying (2020) [207]
Zhao et al.
(Y0.2Nd0.2Sm0.2Eu0.2Er0.2)AlO3 Powder Perovskite Co-precipitation Thermal properties
(2020) [147]
Solution combustion
Phase stability by Bhaskar et al.
(MgNiCoCuZn)O Powder Rock-salt and solid-state
experiments and (2020) [243]
reaction
(continued on next page)

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Table A1 (continued )
Ceramic Composition Sample Crystal Structure Synthesis Method Investigated Properties Reference
Shape

molecular dynamics
simulations
Ce/Gd/La/Nd/Pr/Sm/Y-O Pellet Cubic & Solid-state reaction Phase analysis Pianassola et al.
Monoclinic & pressing (2020) [407]
I. (Co0.2Cu0.2Mg0.2Ni0.2Zn0.2)O I. Rock-salt Chemical and
Solution combustion Xiang et al.
II. (Cr0.2Fe0.2Mn0.2Mg0.2Zn0.2)3O4 Powder II. Spinel microstructural
synthesis (2020) [111]
III. (Ce0.2La0.2Pr0.2Sm0.2Y0.2)O2 III. CaF2-type homogeneity
Hydrothermal Application in Li-ion Nguyen et al.
Cr,Mn,Fe,Co,Ni-O Powder Spinel
method battery (2020) [533]
Sharma et al.
La(Cr0.2Mn0.2Fe0.2Co0.2Ni0.2)O3 Film Perovskite Solid-state reaction Magnetic properties
(2020) [152]
BaZr0.2Sn0.2Ti0.2Hf0.2Ce0.2O3-δ, BaZr0.2Sn0.2Ti0.2Hf0.2Y0.2O3-δ,
Gazda et al.
BaZr1/7Sn1/7Ti1/7Hf1/7Ce1/7Nb1/7Y1/7O3-δ Powder Perovskite Solid-state reaction Proton conductivity
(2020) [549]
BaZr0.15Sn0.15Ti0.15Hf0.15Ce0.15Nb0.15Y0.10O3-δ
Reverse co- Sarkar et al.
(Ce0.2La0.2Pr0.2Sm0.2Y0.2)O2− Powder Fluorite Band structure
precipitation (2020) [565]
δ

Droplet-to-particle Wang et al.

Au/Co/Cu/Ir/Pt/Mn/Mo/Ni/Pd/Ru-O Powder Optimizing synthesis
aerosol (2020) [381]
Musicó et al.
HEOs Review on approaches to compositional design
(2020) [37]
Dielectric and energy Liu et al. (2020)
(Bi0.2Na0.2K0.2Ba0.2Ca0.2)TiO3 Bulk Perovskite Flash sintering
storage properties [145]
Ball-mill & Xu et al. (2020)
(CeZrHfTiLa)Ox Powder Fluorite Catalysis
calcination [466]
Fracchia et al.
(Co,Mg,Mn,Ni,Zn)(Al,Co,Cr,Fe,Mn)2O4 Powder Spinel Solid-state reaction Structural features
(2020) [173]
Lix(M1M2M3M4M5…Mn)O2 Nebulized spray Wang et al.
Powder α-NaFeO2-type Li ion conductivity
(M = Ni, Co, Mn, Al, Fe, Zn, Cr, Ti, Zr, Cu) pyrolysis (2020) [545]
High pressure
Monoclinc + Photocatalytic water Edalati et al.
TiZrHfNbTaO11 Powder torsion & crushing &
Orthorhombic splitting (2020) [297]
annealing
Sarkar et al.
HEOs Review on significance of entropy, enthalpy and synergy on phase stability
(2020) [35]
Application in Na-ion Zhao et al.
NaNi0.12Cu0.12Mg0.12Fe0.15Co0.15Mn0.1Ti0.1Sn0.1Sb0.04O2 Powder O3-type Solis-state reaction
batteries (2020) [546]
Application in Li-ion Lokcu et al.
(MgCoNiZn)1-xLixO Pellet Rock-salt Ball mill & sintering
batteries (2020) [523]
Albedwawi et al.
HEOs Review on catalytic activity
(2021) [457]
(NiFeMnCrCo)xOy
Nebulized spray Application in Li-ion Wang et al.
(NiFeMnCrMg)xOy Powder Spinel
pyrolysis batteries (2020) [548]
(NiFeMnZnMg)xOy
Guo et al.
(La0.2Nd0.2Sm0.2Eu0.2Gd0.2)2Zr2O7 Pellet Pyrochlore Sintering Structural features
(2021) [301]
Corrosion resistance and Wright et al.
[Hf(1− 2x)/3Zr(1− 2x)/3Ce(1− 2x)/3YxYbx]O2-δ (x = 0.2, 0.074, 0.029) Pellet Fluorite Ball mill & sintering
thermal expansion (2021) [446]
Sushil et al.
(Mg,Co,Ni,Cu,Zn)O Powder Rock-salt Auto-combustion Structural features
(2021) [355]
Solution combustion Thermodynamic Saghir et al.
(Co,Mg,Ni,Cu,Zn)O Powder Rock-salt
synthesis evaluation (2021) [354]
Shu et al. (2021)
Ce0.5Zn0.1Co0.1Mg0.1Ni0.1Cu0.1Ox Powder Fluorite Solid-state reaction Catalysis
[505]
Sarkar et al.
HEOs Review on magnetic properties
(2021) [552]
Cormack et al.
HEOs Review on thermodynamic stability
(2021) [33]
Spiridigliozzi
(Ce/Zr/Y/Yb/La/Gd/Sm/Nd/Pr/Ho)-O Descriptor-property relation by computation et al. (2021)
[274]
Cardoso et al.
(Co,Cu,Mg,Ni,Zn)O Resin Rock-salt Polymeric solution Structural stability
(2021) [117]
Thermal conductivity and Zhu et al. (2021)
(Dy0.2Ho0.2Er0.2Y0.2Yb0.2)3NbO7 Pellet Fluorite Ball mill & sintering
mechanical properties [456]
Sol-gel auto- Gautam et al.
(Co0.2Cu0.2Mg0.2Ni0.2Zn0.2)O Powder Rock-salt Crystal Structure
combustion (2021) [408]
[(Sm0.25Eu0.25Gd0.25Yb0.25)2(Ti0.5Hf0.25Zr0.25)2O7]1- Fluorite & Thermomechanical Wright et al.
Pellet Ball mill & sintering
x[(Sc0.266Dy0.248Tm0.246Yb0.240)3NbO7]x Pyrochlore properties (2021) [409]
FCC (< 12.5 at% O)
Reactive magnetron Khan et al.
AlCoCrCu0.5FeNi-O Film Spinel (12.5− 50 at Optimizing synthesis
sputtering (2021) [410]
% O)
Electronic and charge Liang et al.
Ba(Zr0.2Sn0.2Ti0.2Hf0.2Nb0.2)O3 Film Perovskite Sol-gel
transport properties (2021) [411]
Chen et al.
(Ce0.2Zr0.2Ti0.2Sn0.2M0.2)O2-δ Disc Fluorite Ball mill & sintering Crystal structure
(2021) [412]
Ba(Mg0.17Zn0.17Ti0.21Nb0.22W0.23)O3 Disc Perovskite Ball mill & sintering Crystal structure
(continued on next page)

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Table A1 (continued )
Ceramic Composition Sample Crystal Structure Synthesis Method Investigated Properties Reference
Shape

Ba(Mg0.15Yb0.17Ti0.21Nb0.23Ta0.24)O3
Ba(Mg0.16Y0.19Yb0.19Nb0.22W0.24)O3
Ba(Mg0.22Zn0.23Nb0.20W0.17Mo0.18)O3
Ma et al. (2021)
Ba(Mg0.23Yb0.22Ti0.21W0.17Mo0.17)O3
[413]
Ba(Mg0.24Yb0.22Nb0.19Ta0.19W0.16)O3
Ba(Mg0.25Ti0.21Zr0.20Nb0.18W0.16)O3
Ba(Y0.22Yb0.22Dy0.22W0.17Mo0.17)O3
Pyrochlore + Radioactive waste Zhou et al.
(Eu1-xGdx)2(Ti0.2Zr0.2Hf0.2Nb0.2Ce0.2)2O7 Disc Ball mill & sintering
Fluorite management (2021) [414]
Magnetron Sun et al. (2021)
(AlCrFeNiMn)O Film Rock-salt Ferromagnetic property
sputtering [415]
Yang et al.
La0.2Pr0.2Nd0.2Sm0.2Sr0⋅2MnO3-δ Powder Perovskite Sol-gel Solid oxide fuel cell
(2021) [416]
Electrical and thermal Zhang et al.
(La0.2Y0.2Nd0.2Gd0.2Sr0.2)CrO3 Powder Perovskite Sol-gel
conductivity (2021) [417]
Zhang et al.
(CoNiMnZnFe)3O3.2 Powder Rock-salt Ball mill Electrocatalysis
(2021) [418]
Reactive flash Mao et al.
(La0.2Nd0.2Sm0.2Eu0.2Gd0.2)2Zr2O7 Pellet Pyrochlore Ultrafast densification
sintering (2021) [419]
TiO2/ZrO2/SnO2/HfO2,/CeO2/Nb2O5/La2O3/Nd2O3/Sm2O3/ Pyrochlore & Teng et al.
Pellet Ball mill & sintering Structural features
Eu2O3/Gd2O3/Dy2O3/Ho2O3/Er2O3/Tm2O3/Yb2O3/Lu2O3 Fluorite (2021) [420]
Ball mill & spark
plasma sintering, Bonnet et al.
(Hf1/3Ce1/3Zr1/3)1-x(Gd1/2Y1/2)xO2-x/2 Pellet Fluorite Ionic conductivity
precipitation & (2021) [421]
annealing
Ball mill & spark Dupuy et al.
(Cu,Co,Mg,Ni,Zn)O Bulk Rock-salt Microstructural features
plasma sintering (2021) [422]
(La0.2Nd0.2Sm0.2Gd0.2Y0.2)2Ce2O7
(La0.2Nd0.2Gd0.2Er0.2Yb0.2)2Ce2O7
(La0.2Sm0.2Er0.2Yb0.2Y0.2)2Ce2O7 Xu et al. (2021)
Bulk Fluorite Ball mill & sintering Thermal properties
(La0.2Gd0.2Er0.2Yb0.2Y0.2)2Ce2O7 [423]
(Gd0.2Dy0.2Er0.2Yb0.2Y0.2)2Ce2O7
(Sc0.2Er0.2Gd0.2Yb0.2Lu0.2)2Ce2O7
He et al. (2021)
RE2(Ce0.2Zr0.2Hf0.2Sn0.2Ti0.2)2O7 (RE = Y, Ho, Er, Yb) Bulk Fluorite Ball mill & sintering Thermal barrier coating
[424]
(Cr,Mn,Fe,Co,Ni)3O4
Magnetic properties and Cieslak et al.
(Cr,Mn,Fe,Co)3O4 Pellet Spinel Ball mill & sintering
DFT calculation (2021) [425]
(Cr,Mn,Fe,Ni)3O4
Mozdzierz et al.
(Co,Cu,Mg,Ni,Zn)1-x LixO Pellet Cubic Ball mill & sintering Li-ion battery
(2021) [426]
Surfactant-assisted Lithiation/delithiation Huang et al.
Fe-Cr-Co-Ni-Mn-O Powder Spinel
hydrothermal mechanism (2021) [427]
Jin et al. (2021)
(AlCoFeMoCr)3O4 Ribbon Spinel Chemical dealloying Electrocatalysis
[428]
Sharma et al.
(Mg0.2Ni0.2Fe0.2Co0.2Cu0.2)Fe2O4 Film Spinel Pulsed laser epitaxy Magnetic properties
(2021) [429]
Nguyen et al.
La(CrMnFeCo2Ni)O3 Powder Perovskite Precipitation Electrocatalysis
(2021) [430]
Pulsed laser Ahn et al.
(Zr,Hf,Nb,Ta,Mo,W)-O Film Amorphous Memristors
deposition (2021) [431]
Low-temperature Gu et al. (2021)
(FeCrCoNiCu)3O4 Nanosheet Spinel Electrooxidation
plasma strategy [432]
Li et al. (2021)
HEOs Review on electrical properties
[433]
Design of HEOs with
MgO/ZnO/Y2O3/Yb2O3/CeO2/HfO2/ZrO2/SnO2/GeO2/TiO2/ Tang et al.
Disk Perovskite Ball mill & sintering perovskite structure using
Sb2O5/Ta2O5/Nb2O5/Ga2O3/WO3/MoO3 (2021) [434]
valence combination
Magnetic and electrical Zhivulin et al.
(LaNd)(Cr0.2Mn0.2Fe0.2Co0.2Ni0.2)O3 Pellet Perovskite Ball mill & sintering
properties (2021) [435]
Electrical and thermal Zheng et al.
(Ca0.2Sr0.2Ba0.2Pb0.2La0.2)TiO3 Pellet Perovskite Ball mill & sintering
properties (2021) [436]
Ball mill & sintering Zhang et al.
(La0.2Ce0.2Gd0.2Er0.2Tm0.2)2(WO4)3 Powder Monoclinic Radiation shielding
+ mill (2021) [437]

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Table A2
Summary of publications about high-entropy nitrides in chronological order.
Ceramic Composition Sample Crystal Structure Synthesis Method Investigated Properties Reference
Shape

Fe-Co-Ni-Cr-Cu-Al-Mn-N Chen et al. (2004)

Film Amorphous Reactive DC sputtering Mechanical properties
Fe-Co-Ni-Cr-Cu-Al0.5-N [48]
I. AlxCoCrCuFeNi-N Morphology, structure and mechanical Chen et al. (2005)
Film Amorphous Reactive DC sputtering
II. AlCrNiSiTi-N properties [54]
Reactive radio-
Optimizing synthesis (N2 flow rate), Lai et al. (2006)
AlCrTaTiZr-N Film FCC frequency magnetron
microstructure and mechanical properties [629]
sputtering
Reactive radio- Optimizing synthesis (substrate
Lai et al. (2007)
(AlCrTaTiZr)N Film FCC frequency magnetron temperature), crystal structure and
[628]
sputtering mechanical properties
Reactive magnetron Tsai et al. (2008)
(AlMoNbSiTaTiVZr)50N50 Film Amorphous Diffusion barrier characteristics
sputtering [587]
Amorphous, FCC +
Optimizing synthesis (nitrogen flow rate) Tsai et al. (2008)
(AlMoNbSiTaTiVZr)Nx Film Amorphous or FCC Magnetron sputtering
and crystal structure [623]
(depending on N2 flow rate)
Reactive radio-
Thermal stability and thermal barrier Chang et al. (2009)
AlCrTaTiZr-N Film FCC + Amorphous frequency magnetron
performance [656]
sputtering
Reactive radio-
Effect of nitrogen fraction on microstructure Huang et al. (2009)
(AlCrNbSiTiV)N Film FCC frequency magnetron
and mechanical properties [610]
sputtering
Reactive radio- Optimizing synthesis (substrate
Huang et al. (2009)
(AlCrNbSiTiV)N Film FCC frequency magnetron temperature), microstructure and
[631]
sputtering mechanical properties
Huang et al. (2010)
(AlCrNbSiTiV)N Film FCC Reactive sputtering Mechanical properties
[614]
Reactive magnetron Optimizing synthesis (bias), crystal Shen et al. (2012)
(Al1.5CrNb0.5Si0.5Ti)Nx Film FCC
reactive sputtering structure and mechanical properties [621]
Amorphous or FCC
Reactive magnetron Tsai et al. (2012)
(AlBCrSiTi)N Film (depending on annealing Structural features
sputtering [588]
temperature)
Optimizing synthesis (nitrogen content and
Reactive DC Hsueh et al. (2012)
(AlCrSiTiZr)100-xNx Film Amorphous bias) on mechanical properties and
magnetron sputtering [639]
corrosion resistance
Cathode vacuum arc Pogrebnjak et al.
(Ti-Hf-Zr-V-Nb)N Film FCC Elemental and structural analysis
deposition (2013) [589]
Cathodic vacuum arc Pogrebnjak et al.
(TiZrHfVNb)N Film FCC Microhardness and tribological properties
deposition (2013) [590]
TiN
(TiTa)N
Reactive radio-
(TiTaCr)N Application as interdiffusion barrier for Cu Chang et al. (2013)
Film FCC frequency magnetron
(TiTaCrZr)N and Si interface [591]
sputtering
(TiTaCrZrAl)N
(TiTaCrZrAlRu)N
(Al23.1Cr30.8Nb7.7Si7.7Ti30.7)N50 Reactive magnetron Optimizing synthesis (bias), microstructure Hsieh et al. (2013)
Film FCC
(Al29.1Cr30.8Nb11.2Si7.7Ti21.2)N50 sputtering and mechanical properties [609]
Reactive magnetron Shen et al. (2013)
(Al0.34Cr0.22Nb0.11Si0.11Ti0.22)50N50 Film FCC The oxidation resistance
sputtering [640]
Firstov et al.
Ti-V-Zr-Nb-Hf-N Plate FCC Vacuum arc deposition Mechanical properties and thermal stability
(2014) [617]
Cathodic arc vapor Crystal structure, distribution of defects and Pogrebnjak et al.
(Ti-Hf-Zr-V-Nb)N Film FCC
deposition strain analysis (2014) [615]
Pogrebnjak et al.
HENs Review on crystal structure and properties
(2014) [592]
Reactive magnetron Shen et al. (2015)
(Al0.34Cr0.22Nb0.11Si0.11Ti0.22)50N50 Film FCC Mechanical and thermal properties
sputtering [613]
Nyemchenko et al.
(TiZrHfVNbTa)N Coating FCC Vacuum arc deposition Optimizing synthesis (nitrogen pressure)
(2015) [619]
Gorban et al.
TiZrHfVNbTa-N Disk FCC Vacuum arc spraying Tribological properties
(2016) [594]
I. (Zr-Ti-Nb)N Film I: FCC
Pogrebnjak et al.
II. (Zr-Ti-Cr-Nb)N II: FCC + Trigonal Vacuum arc deposition Tribological properties
(2017) [618]
III. (Zr-Ti-Cr-Nb-Si)N III: FCC
Bagdasaryan et al.
(TiZrNbHfTa)N/MoN Film FCC Vacuum arc deposition Phase composition, texture and hardness
(2017) [620]
Filtered cathodic Vereschaka et al.
Ti-TiN-(ZrNbTi)N Coating Multi-phases Mechanical strength and wear resistance
vacuum arc deposition (2017) [595]
Reactive DC Effect of atomic size difference on hardness Zhang et al. (2018)
(Al0.5CrFeNiTi0.25)Nx Film FCC
magnetron sputtering and elastic modulus [382]
Effect of processing bias on structure and Sobol et al. (2018)
(FeCoNiCuAlCrV)N Film FCC Vacuum arc deposition
mechanical properties [622]
Reactive DC Mechanical properties and electrical Johansson et al.
Hf-Nb-Ti-V-Zr-N Film FCC (0− 07 at% Hf)
magnetron sputtering resistivity (2018) [630]
(continued on next page)

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Table A2 (continued )
Ceramic Composition Sample Crystal Structure Synthesis Method Investigated Properties Reference
Shape

FCC + Tetragonal (10− 18 at

% Hf)
V-Cr-Nb-Mo-Zr-N Powder Cubic Soft urea method Electrochemical properties for Jin et al. (2018)
supercapacitors [372]
(TiZrNbHfTa)N/WN Coating FCC Vacuum arc Structural and mechanical characterization Bagdasaryan et al.
evaporation (2018) [637]
(NbTiAlSiZr)Nx Film Amorphous or FCC Magnetron sputtering Mechanical properties and thermal stability Xing et al. (2018)
(depending on annealing [626]
temperature)
(TiVCrZrNbMoHfTaWAlSi)N Film Amorphous, FCC or HCP + DC magnetron Influence of nitrogen flow rate on crystal Chang et al. (2018)
FCC (depending on N2 flow sputtering structure [625]
rate)
(Al,Ta,Ti,V,Zr)N Film FCC Magnetron sputtering Micromechanical properties Hahn et al. (2019)
[638]
(AlCrTaTiZrMo)N Film Amorphous Reactive DC Thermal stability for diffusion barriers Li et al. (2019)
magnetron sputtering [385]
CoCrFeMnNi-N Film FCC or CrN-type (depending Plasma nitriding Mechanical properties and corrosion Nishimoto et al.
on temperature) resistance (2019) [633]
(AlCrNbSiTiV)N Film FCC Reactive DC Optimizing synthesis and mechanical Chang et al. (2019)
magnetron sputtering properties [624]
(TiZrNbVHf)N Sobol et al. (2019)
Film FCC Vacuum arc deposition Optimizing synthesis
(TiZrNbVHfTa)N [597]
(AlCrVFeCoNiCu)N
(AlCrTiNbSi)N Sobol et al. (2019)
Film FCC Vacuum arc deposition Optimizing synthesis
(AlCrTiZrNbV)N [636]
(TiZrNbVHf)N
FCC (for optimized N2 flow Reactive magnetron Kirnbauer et al.
(Hf,Ta,Ti,V,Zr)N Film Mechanical properties
rate) sputtering (2020) [268]
Reactive DC Effect of synthesis on microstructure and Kim et al. (2020)
AlCoCrNi-N Film Amorphous
magnetron sputtering mechanical properties [598]
Amorphous + FCC or Reactive radio- Influence of processing bias on structure,
Wang et al. (2020)
(AlCrSiNbZr)Nx Film Amorphous (depending on frequency magnetron morphology, hardness and electrical
[627]
substrate bias) sputtering resistivity
Influence of nitriding on microstructure and Chen et al. (2020)
(VAlTiCrMo)Nx Coating FCC Magnetron sputtering
mechanical properties [384]
Amorphous (0 at% N)
FCC + Amorphous (15− 41 at Reactive DC Effect of nitrogen fraction on crystal Fieandt et al.
Al-Cr-Nb-Y-Zr-N Film
% N) magnetron sputtering structure and mechanical properties (2020) [383]
FCC (46–51 at% N)
Reactive DC Influence of substrate temperatures and bias Fieandt et al.
(Al,Cr,Nb,Y,Zr)N Film FCC
magnetron sputtering on corrosion and mechanical properties (2020) [632]
Lewin et al. (2020)
HENs Review on properties for coating applications
[84]
Lin et al. (2020)
(Cr0.35Al0.25Nb0.12Si0.08V0.20)N Film FCC Magnetron sputtering Mechanical properties
[612]
Cui et al. (2020)
(AlCrTiZrHf)N Film FCC Magnetron sputtering Mechanical properties
[611]
Mechanical
Moskovskikh et al.
(Hf0.2Nb0.2Ta0.2Ti0.2Zr0.2)N Film FCC combustion & spark Mechanical properties
(2020) [616]
plasma sintering
(HfNbTaTiZr) Nx
(CrNbTaTiV)Nx
(CrHfNbTaTi)Nx
(CrHfNbTiZr)Nx
(CrHfTaTiZr)Nx
Ball mill & spark Dippo et al. (2020)
(HfNbTaTiZr)(CN)x Pellet FCC Mechanical properties
plasma sintering [634]
(CrNbTaTiV)(CN)x
(CrHfNbTaTi)(CN)x
(CrHfNbTiZr) (CN)x
(CrHfTaTiZr) (CN)x
(CrMoTaVW) (CN)x
FCC + BCC or, Amorphous Mechanical properties and oxidation Khan et al. (2020)
AlCoCrCu0.5FeNi Film Magnetron sputtering
(depending on N2 flow rate) behavior [635]
He et al. (2021)
AlCrTaTiZrN Film Amorphous Magnetron sputtering Solar absorption
[659]
Wang et al. (2021)
Al-Cr-Nb-Si-Zr-N Film Amorphous Magnetron sputtering Oxidation behavior
[599]
Lu et al. (2021)
(CrAlTiNbV)Nx Film FCC Magnetron sputtering Anti-wear applications
[601]
Influence of voltage on composition, Xu et al. (2021)
(AlCrTiVZr)N Film FCC Magnetron sputtering
microstructure and mechanical properties [600]
FCC (x = 0) Yu et al. (2021)
(AlCrTiZrMo)-Six-N Film Magnetron sputtering Mechanical behavior
Amorphous (x > 0) [602]
BCC (low nitrogen flow) Xia et al. (2021)
(MoNbTaVW)1-xNx Film
FCC (high nitrogen flow) [603]
(continued on next page)

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Table A2 (continued )
Ceramic Composition Sample Crystal Structure Synthesis Method Investigated Properties Reference
Shape

Magnetron sputtering Effect of nitrogen on structure, composition,

& cathodic arc mechanical properties and electrical
deposition properties
Amorphous (10 at% N) Influence of nitrogen on microstructure and
Bachani et al.
TiZrNbTaFeN Film Magnetron sputtering tribological, electrical, mechanical and
FCC (> 10 at% N) (2021) [604]
corrosion properties
Reactive magnetron Zaid et al. (2021)
(VNbTaMoW)N/Al2O3 Film Cubic Elastic modulus
sputtering [605]
Amorphous (as-deposited)
BCC (Anneal with > 0.5 at% Radio-frequency Kao et al. (2021)
TaNbSiZrCr-N Film Mechanical and thermal properties
N) magnetron sputtering [606]
FCC (Anneal 0.5 at% N)
Huang et al. (2021)
Al/Si/Ti/V/Cr/Zr/Nb/Mo-N Single phase prediction using DFT calculations
[233]
Casting & plasma Lan et al. (2021)
Ni45(CoCrFe)40(AlTi)15-N Ingot Multi-phases Wear behavior
nitriding [608]
Amorphous (< 50 at% N) Xu et al. (2021)
(TiCrZrVAl)N Film Multi-arc ion plating Mechanical and tribological properties
FCC (> 50 at% N) [607]
Radio-frequency Guo et al. (2021)
AlCrMoTaTiN/Al2O3 Film Multi-phases Solar absorption
reactive sputtering [660]
Radio-frequency
Zhao et al. (2021)
Al0.4Hf0.6NbTaTiZrN/Al2O3 Film FCC reactive magnetron Solar absorption
[661]
sputtering
He et al. (2021)
AlCrWTaNbTiN/Al2O3 Film Amorphous & FCC Magnetron sputtering Solar absorption
[662]
Reactive magnetron He et al. (2021)
AlCrTaTiZrN/Al2O3 Film Amorphous Solar absorption
sputtering [663]

Table A3
Summary of publications about high-entropy carbides in chronological order.
Ceramic Composition Sample Crystal Structure Synthesis Method Investigated Properties Reference
Shape

(TiAlCrNbY)C Film FCC Magnetron sputtering Mechanical properties Braic et al. (2010)
[59]
(TiZrNbHfTa)C Film FCC Co-sputtering Biocompatibility Braic et al. (2012)
[692]
(TiZrNbHfTa)C Film FCC Co-sputtering Texture, microstructure, hardness, Braic et al. (2012)
friction and wear resistance [690]
(CuSiTiYZr)C Film Amorphous Co-sputtering Mechanical properties and Braic et al. (2013)
corrosion resistance [719]
(CrCuNbTiY)C Film FCC Co-sputtering Mechanical properties and Braic et al. (2014)
tribological performance [720]
(TiZrNbTaHf)C Film cubic Magnetron sputtering Biocompatibility Vladescu et al. (2016)
[388]
FeCoCrNiMn-C Ingot FCC + Intermetallics Arc melting Mechanical properties Cheng et al. (2017)
[724]
(Hf-Ta-Zr-Nb)C Bulk FCC Ball mill & spark plasma Microstructure characterization Dusza et al. (2018)
sintering [664]
(Ti,Zr,Hf,Nb,Ta)C Powder FCC Ball mill & spark plasma Crystal structure and oxidation Zhou et al. (2018)
sintering & crushing behavior [726]
(TaNbHfTiZr)C Structure, mechanical properties and electronic structure by experiments and DFT calculations Yang et al. (2018)
[212]
HfC/NbC/TaC/TiC/Mo2C/VC/ Pellet Rock-salt Ball mill & spark plasma Synthesizability and hardness Sarker et al. (2018)
W2C/ZrC sintering [267]
(Hf0.2Zr0.2Ta0.2Nb0.2Ti0.2)C Pellet Rock-salt Spark plasma sintering Thermal conductivity Yan et al. (2018)
[313]
(Hf-Ta-Zr-Ti)C Ball mill & spark plasma Castle et al. (2018)
Bulk Rock-salt Mechanical properties
(Hf-Ta-Zr-Nb)C sintering [686]
Densification behavior and Feng et al. (2019)
(Hf,Zr,Ti,Ta,Nb)C Powder Rock-salt Carbothermal reduction
mechanical properties [340]
I. (HfMoTaTi)C I. FCC Ball mill & spark plasma Optimizing synthesis and Zhang et al. (2019)
Pellet
II. (HfMoTaTiB)C II. Hexagonal sintering mechanical properties [666]
Gao et al. (2019)
CrMnFeCoNi-C Sheet FCC + NbC-type Arc melting Mechanical properties
[667]
Ball mill & spark plasma Microstructures and elemental Wei et al. (2019)
(Ti0.2Zr0.2Nb0.2Ta0.2W0.2)C Bulk Rock-salt
sintering distribution [314]
I. Bulk I. Ball mill & sintering
Chen et al. (2019)
(Zr0.2Hf0.2Ti0.2Nb0.2Ta0.2)C bar Rock-salt II. Gas-released in-situ reaction & Thermal and mechanical properties
[722]
sintering
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Table A3 (continued )
Ceramic Composition Sample Crystal Structure Synthesis Method Investigated Properties Reference
Shape

II. Porous
bar
(Ta-Hf-Zr-Nb)C Bulk FCC Ball mill & spark plasma Creep behavior Han et al. (2019)
sintering [669]
(Zr,Nb,Hf,Ta)C Foil cubic Spark plasma sintering Microstructural features Biesuz et al. (2019)
[670]
(Zr0.25Nb0.25Ti0.25V0.25)C Pellet Rock-salt Ball mill & sintering Structure and mechanical Ye et al. (2019) [258]
properties by experiments and DFT
calculations
I. (Ti0.2Zr0.2Hf0.2Nb0.2Ta0.2)C I-IX. Rock-salt
II. (Ti0.2Hf0.2V0.2Nb0.2Ta0.2)C
III. (Ti0.2V0.2Nb0.2Ta0.2W0.2)C
IV. (Ti0.2Zr0.2Hf0.2Ta0.2W0.2)C
V. (Ti0.2Hf0.2Nb0.2Ta0.2W0.2)C
VI. (Ti0.2V0.2Nb0.2Ta0.2Mo0.2)C Ball mill & spark plasma Harrington et al.
Pellet Mechanical properties
VII. (Ti0.2Zr0.2Hf0.2Ta0.2Mo0.2)C X-XII. Multi-phases sintering (2019) [275]
VIII. (Ti0.2Hf0.2Nb0.2Ta0.2Mo0.2)C
IX. (V0.2Nb0.2Ta0.2Mo0.2W0.2)C
X. (Zr0.2Hf0.2Ta0.2Mo0.2W0.2)C
XI. (Ti0.2Zr0.2Hf0.2Mo0.2W0.2)C
XII. (Zr0.2Hf0.2V0.2Mo0.2W0.2)C
Mechanical properties and
Zhang et al. (2019)
B4(HfMo2TaTi)C + SiC Bulk HCP Pulsed current processing oxidation behavior by experiments
[260]
and DFT calculation
Chicardi et al. (2019)
(TiZrHfVNb)C5 Powder FCC Ball mill Microstructural features
[671]
Nano-
(Ti0.2Zr0.2Hf0.2Nb0.2Ta0.2)C FCC Carbothermal reduction Microstructural features Li et al. (2019) [339]
powder
(Hf0.2Ta0.2Ti0.2Nb0.2Mo0.2)C Sedegov et al. (2019)
Powder FCC Various solid-state methods Optimizing synthesis
(Hf0.2Ta0.2Ti0.2Nb0.2Zr0.2)C [672]
Electronic structure and mechanical
Ball mill & spark plasma Zhang et al. (2019)
(TiZrHfNbTa)C Pellet FCC properties by experiments and DFT
sintering [259]
calculations
Ball mill & spark plasma Csanádi et al. (2019)
(Hf-Ta-Zr-Nb)C Bulk FCC Mechanical properties
sintering [673]
Ball mill & spark plasma Wang et al. (2020)
(Hf0.2Ta0.2Zr0.2Ti0.2Nb0.2)C-xSiC Pellet Rock-salt Oxidation behavior
sintering [322]
I. Hf0.2Ta0.2Ti0.2Nb0.2Zr0.2C Ball mill & spark plasma Moskovskikh et al.
Bulk FCC Thermal and mechanical properties
II. Hf0.2Ta0.2Ti0.2Nb0.2Mo0.2C sintering (2020) [283]
Ball mill & spark plasma Tan et al. (2020)
(Zr,Ti,Hf,Nb,Ta)C Bulk Rock-salt Oxidation behaviors
sintering [323]
Wei et al. (2020)
(Ti0.2Hf0.2Nb0.2Ta0.2W0.2)C Pellet FCC Reactive spark plasma sintering Gradient microstructural evolution
[265]
I. (Ti0.2Zr0.2Hf0.2Nb0.2Ta0.2)C I. Multi-phases
Ball mill & spark plasma
II. (Ti0.2Zr0.2Hf0.2Nb0.2Ta0.2)C + 20 Disk Mechanical properties Lu et al. (2020) [712]
II. FCC sintering
vol% SiC
Ball mill & spark plasma Liu et al. (2020)
(VNbTaMoW)C Powder Rock-salt Crystal structure
sintering [715]
Microstructure and mechanical Wang et al. (2020)
(TiZrNbTaMo)C Powder FCC Carbothermal
properties [682]
(Hf0.2Zr0.2Ta0.2Nb0.2Ti0.2)C Pellet Ball mill & hot-press sintering Oxidation behavior Ye et al. (2020) [303]
Ball mill & spark plasma Csanádi et al. (2020)
(Hf-Ta-Zr-Nb)C Bulk Cubic Fracture behavior during bending
sintering [674]
(HfTaZrTi)C Jiang et al. (2020)
Elastic and thermodynamic features by DFT calculations
(HfTaZrNb)C [85]
(NbTaZr)C
(NbTaTiZr)C
Zhao et al. (2020)
(NbTiVZr)C Lattice distortion evaluation by DFT calculations
[262]
(HfNbTaTiZr)C
(MoNbTaVW)C
Kan et al. (2020)
(Ti,Zr,Nb,Ta,Hf)C Foil Multi-cubic phases Arc melting Use as hard precipitates in steels
[714]
Ball mill & spark plasma Peng et al. (2020)
TiC0.4/WC/0.5 Mo2C Bulk Rock-salt Mechanical properties
sintering [716]
Ball mill & spark plasma Effect of vacancies on interfacial
NbC0.5-MC (M = V, Ti, Ta, W) Bulk Rock-salt He et al. (2020) [675]
sintering diffusion
V2(Sn, A)C (A = Fe, Co, Ni, Mn) Powder Hexagonal MAX phase Alloy-guided reaction Magnetic properties Li et al. (2020) [693]
Nano- Ning et al. (2020)
(Ta0.25Nb0.25Ti0.25V0.25)C Rock-salt Molten salt synthesis Optimizing synthesis
powder [276]
(Hf0.25Nb0.25Zr0.25Ti0.25)C Powder Rock-salt Polymer-derived ceramic route Optimizing synthesis Du et al. (2020) [676]
Sure et al. (2020)
(TiNbTaZrHf)C Powder FCC Facile electrochemical method Structural analysis
[368]
Dai et al. (2020)
(Zr0.2Hf0.2Ti0.2Nb0.2Ta0.2)C Prediction of thermal and mechanical properties by machine learning
[228]
Nb/Hf/Ti/Zr/V/Ta/Mo/W/Cr-C Bulk FCC or multi-phases
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Table A3 (continued )
Ceramic Composition Sample Crystal Structure Synthesis Method Investigated Properties Reference
Shape

Ball mill & spark plasma Predicting synthesizability by Kaufmann et al.

sintering machine learning and experiments (2020) [266]
(Hf0.2Zr0.2Ta0.2Nb0.2Ti0.2)C Bulk Rock-salt Ball mill & spark plasma Thermal and mechanical properties Wang et al. (2020)
sintering [713]
(Ti,Zr,Hf,Ta,La,Y)C
Sun et al. (2020)
(Ti,Zr,Hf,Ta,Nb,La,Y)C Powder FCC Polymeric precursor synthesis Structural analysis
[375]
(Ti,Zr,Hf,Ta,Nb,Mo,W,La)C
TiZrHfVNbC5
TiZrHfVTaC5
TiZrHfNbTaC5 Chicardi et al. (2020)
Powder FCC Ball mill Optimizing synthesis
TiZrVNbTaC5 [281]
TiHfVNbTaC5
ZrHfVNbTaC5
(Ti,Zr,Hf,V,Nb,Ta, ×,Y)C (X,Y = Wang et al. (2020)
Mechanical properties by DFT calculations
Mo, W, Cr, Mo, Cr, W) [718]
Zhao et al. (2020)
Al-Ti-V-Nb-Ta-C Pellet Rock-salt Ball mill & sintering Structural analysis
[282]
Hf0.2Zr0.2Ta0.2Mo0.2W0.2C1-x Rost et al. (2020)
Film Rock-salt Sputtering deposition Thermal conductivity
Hf0.2Zr0.2Ta0.2Ti0.2Nb0.2C1-x [723]
Zhou et al. (2021)
(Ti0.2Zr0.2Hf0.2Nb0.2Ta0.2)C Powder Rock-salt Carbothermal reduction Electromagnetic wave absorption
[738]
Carbothermal reduction & hot Feng et al. (2021)
(Hf,Zr,Ti,Ta,Nb)C Pellet Rock-salt Mechanical properties
pressing [717]
Wei et al. (2021)
Re0.5MoNbW(TaC)0.8 Ingot Multi-phases Arc melting Mechanical properties
[694]
Guan et al. (2021)
(Ti0.2Zr0.2Nb0.2Ta0.2Mo0.2)C Powder Cubic Ball mill & heat treatment Phase stability
[695]
̌
Solcová et al. (2021)
(Ti,Zr,Hf,Ta,Nb)-C Powder Cubic Xerogel treatment Optimizing synthesis
[696]
BCC + HCP or Rock-salt
Reactive radio-frequency Hossain et al. (2021)
(HfNbTaTiZr)Cx Film (depending on methane Mechanical properties
magnetron sputtering [697]
flow)
Densification and mechanical Sun et al. (2021)
(Hf0.2Ta0.2Zr0.2Nb0.2Ti0.2)C Disc Rock-salt Ball mill & hot pressing
properties [698]
Carbothermal reduction, ball Thermal conductivity and Wei et al. (2021)
(Ti0.2Zr0.2Hf0.2Nb0.2Ta0.2)C Pellet Dual FCC phases
milling & spark plasma sintering mechanical properties [699]
Theorical and experimental
Reactive radio-frequency Wang et al. (2021)
(CrNbSiTiZr)C Film Cubic investigation of tribological and
magnetron sputtering [700]
corrosion properties
Amorphous (low C2H2
Tribological, mechanical, anti-glass
flow rate) Radio-frequency magnetron Kao et al. (2021)
TaNbSiZrCr-C Film sticking and anti-corrosion
FCC (high C2H2 flow sputtering [701]
properties
rate)
(Hf-Ta-Ti-Nb-V)C-19.2 vol% Co Pötschke et al. (2021)
Bar Cubic Ball mill & gas pressure sintering Physical and mechanical properties
(Ta-Ti-Nb-V-W)C-19.2 vol% Co [702]
Ball mill & two-step spark plasma Tribological and mechanical Dusza et al. (2021)
(Hf-Ta-Zr-Nb-Ti)C Pellet Rock-salt
sintering properties [703]
Ball mill & reactive spark plasma Mechanical, thermal and electrical Vasanthakumar et al.
(Ti0.2W0.2Ta0.2Mo0.2V0.2)C0.8 Pellet Rock-salt
sintering properties (2021) [704]
Ball mill & spark plasma Wang et al. (2021)
(Hf0.2Ta0.2Zr0.2Ti0.2Nb0.2)C Pellet Rock-salt Oxidation behavior
sintering [705]
(NbTaZr)C
(NbTaZrW)C Ball mill & spark plasma Mechanical and electronic
Bulk Rock-salt Li et al. (2021) [706]
(ZrNbTaHf)C sintering properties
(NbTaZrHfW)C
(Hf,Ta,Nb,Ti,V)C Ball mill, gas pressure sintering,
Densification and mechanical Potschke et al. (2021)
Plate Cubic vacuum sintering & spark plasma
(Ta,Nb,Ti,V,W)C properties [707]
sintering
(Hf0.2Zr0.2Ta0.2Nb0.2Ti0.2)C Billet FCC Ball mill & sintering Mechanical and thermal properties Yu et al. (2021) [708]
Ball mill & spark plasma Tribological and mechanical Sun et al. (2021)
(Hf0.2Mo0.2Nb0.2Ta0.2Ti0.2)C Bulk Rock-salt
sintering properties [709]
(Ti,Zr,Hf,Ta,W)C Sangiovanni et al.
Investigate of elastic properties by molecular dynamic simulation
(V,Nb,Ta,Mo,W)C (2021) [234]
(HfTaTiWZr)C Ball mill & spark plasma Sangiovanni et al.
Pellet Cubic Plasticity
(MoNbTaVW)C sintering (2021) [710]
FCC + C phase + SiC Precursor infiltration and Mechanical properties and ablation Cai et al. (2021)
Cf/(Ti0.2Zr0.2Hf0.2Nb0.2Ta0.2)C-SiC Powder
phase pyrolysis resistance [711]

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Table A4
Summary of publications about high-entropy borides in chronological order.
Ceramic Composition Sample Crystal Structure Synthesis Method Investigated Properties Reference
Shape

(Hf0.2Zr0.2Ta0.2Nb0.2Ti0.2)B2
(Hf0.2Zr0.2Ta0.2Mo0.2Ti0.2) B2
(Hf0.2Zr0.2Mo0.2Nb0.2Ti0.2)B2 Ball mill & spark plasma Gild et al. (2016)
Disk Hexagonal Hardness and oxidation resistance
(Hf0.2Mo0.2Ta0.2Nb0.2Ti0.2)B2 sintering [86]
(Mo0.2Zr0.2Ta0.2Nb0.2Ti0.2)B2
(Hf0.2Zr0.2Ta0.2Cr0.2Ti0.2)B2
Magnetron sputtering Mayrhofer et al.
Zr0.23Ti0.20Hf0.19V0.14Ta0.24B2 Film Hexagonal Hardness and microstructure
deposition (2018) [387]
Wang et al.
(Hf0.2Zr0.2Ta0.2M0.2Ti0.2)B2 (M = Nb, Mo, Cr) Mechanical properties and electronic structure by DFT calculations
(2018) [269]
Liu et al. (2019)
(Hf0.25Ta0.25Nb0.25Ti0.25)B2 Powder Hexagonal Borocarbothermal reduction Optimizing synthesis
[336]
Reactive flash spark plasma Gild et al. (2019)
(Hf0.2Zr0.2Ta0.2Nb0.2Ti0.2)B Pellet Hexagonal Structural analysis
sintering [309]
(Hf0.2Zr0.2Ta0.2Cr0.2Ti0.2)B2
Ball mill & spark plasma Crystal structure, microstructure Zhang et al.
(Hf0.2Mo0.2Zr0.2Nb0.2Ti0.2)B2 Bulk Hexagonal
sintering and Vickers hardness (2019) [586]
(Hf0.2Mo0.2Ta0.2Nb0.2Ti0.2)B2
Liu et al. (2019)
(Hf0.2Zr0.2Ta0.2Nb0.2Ti0.2)B2 Powder Hexagonal Borothermal reduction Phase formation mechanism
[332]
(Hf0.2Zr0.2Ta0.2Nb0.2Ti0.2)B2
Borocarbothermal reduction Crystal structure, microstructure Zhang et al.
(Hf0.2Zr0.2Mo0.2Nb0.2Ti0.2)B2 Disk Hexagonal
& spark plasma sintering and Vickers hardness (2019) [334]
(Hf0.2Mo0.2Ta0.2Nb0.2Ti0.2)B2
Ball mill & spark plasma Shen et al.
(Ti0.2Zr0.2Hf0.2Nb0.2Ta0.2)B2-SiC Bulk Hexagonal Mechanical properties
sintering (2019) [311]
Borocarbothermal reduction Gu et al. (2019)
(Ti0.2Hf0.2Zr0.2Nb0.2Ta0.2)B2 Bulk Hexagonal Crystal structure and morphology
& spark plasma sintering [338]
Borocarbothermal reduction Chen et al.
(Zr0.2Hf0.2Ti0.2Nb0.2Ta0.2)B2 Bulk Hexagonal Mechanical and thermal properties
& partial sintering (2019) [341]
Self-propagating high- Compositional and structural Tallarita et al.
(Hf0.2Mo0.2Ta0.2Nb0.2Ti0.2)B2 Bulk Hexagonal
temperature synthesis characterization (2019) [347]
(Zr0.2Ta0.2Ti0.2Nb0.2Hf0.2)B2 Borothermal reduction & Crystal structure, microstructure Zhang et al.
Bulk Hexagonal
(Zr0.2W0.2Ti0.2Mo0.2Hf0.2)B2 spark plasma sintering and hardness (2020) [331]
(Hf0.2Zr0.2Ti0.2Ta0.2Nb0.2)B2
(Hf0.2Zr0.2Ti0.2Ta0.2Mo0.2)B2 Borocarbothermal reduction Gild et al. (2020)
Disk Hexagonal Mechanical and thermal properties
(Hf0.2Zr0.2Ti0.2Ta0.2Cr0.2)B2 & spark plasma sintering [333]
(Hf0.2Zr0.2Ti0.2Mo0.2W0.2)B2
Ball mill & non-reactive or
Hexagonal or Optimizing synthesis and oxidation Tallarita et al.
(Hf0.2Mo0.2Zr0.2Nb0.2Ti0.2)B2 Bulk reactive spark plasma
Multi-phases resistance (2020) [324]
sintering
(Ti0.2Zr0.2Hf0.2Mo0.2W0.2)B2
(Ti0.2Ta0.2Cr0.2Mo0.2W0.2)B2
(Zr0.2Hf0.2Nb0.2Ta0.2W0.2)B2 Reactive spark plasma Microstructure and Vickers Qin et al. (2020)
Pellet Hexagonal
(Zr0.225Hf0.225Ta0.225Mo0.225W0.1)B2 sintering microhardness [300]
(Ti0.2Zr0.2Hf0.2Nb0.2Ta0.2)B2
(Ti0.2Zr0.2Nb0.2Ta0.2Mo0.2)B2
Borocarbothermal reduction Optimizing synthesis and Feng et al.
(Hf0.2,Zr0.2,Ti0.2,Ta0.2,Nb0.2)B2 Bulk Hexagonal
& spark plasma sintering microstructure (2020) [326]
(Zr0.25Ta0.25Nb0.25Ti0.25)B2
(Hf0.25Ta0.25Nb0.25Ti0.25)B2 Nano- Molten-salt-mediated Crystal structure, microstructure Ye et al. (2020)
Hexagonal
(Hf0.25Zr0.25Ta0.25Nb0.25)B2 powder magnesiothermic reduction and homogeneity [743]
(Ta0.25Nb0.25Ti0.25Cr0.25)B2
Feng et al.
(Hf,Zr,Ti,Ta,Nb)B2 Powder Hexagonal Borocarbothermal reduction Optimizing synthesis
(2020) [337]
(Ti0.2Zr0.2Hf0.2Nb0.2Ta0.2)B2 Microstructure and mechanical Liu et al. (2020)
Pellet Hexagonal Ball mill & hot pressing
(Ti0.2Zr0.2Hf0.2Nb0.2Ta0.2)B2 + 20 vol% SiC properties [744]
(Hf0.2,Zr0.2,Ti0.2,Ta0.2,Cr0.2)B2
(Hf0.25,Zr0.25,Ti0.25,Ta0.25)B2
Optimizing synthesis and
(Hf0.25,Zr0.25,Ti0.25,Cr0.25)B2 Failla et al.
Pellet Hexagonal Arc melting microhardness for application as
(Hf0.25,Zr0.25,Cr0.25,Ta0.25)B2 (2020) [746]
ultra-high temperature ceramics
(Hf0.25,Cr0.25,Ti0.25,Ta0.25)B2
(Cr0.25,Zr0.25,Ti0.25,Ta0.25)B2
Liu et al. (2020)
(Ta0.2Nb0.2Ti0.2W0.2Mo0.2)B2 Powder Hexagonal Facile molten salt method Optimizing synthesis
[277]
Bulk Effect of synthesis on porosity,
Chen et al.
(Y0.2Yb0.2Sm0.2Nd0.2Eu0.2)B6 columnar Cubic Solid-state reaction permeability and mechanical
(2020) [747]
shape strength
Borocarbothermal & hot Monteverde et al.
(Hf,Nb,Ta,Ti,Zr)B2 Pellet Hexagonal Mechanical properties
pressing (2020) [745]
(Hf0.2Zr0.2Mo0.2Nb0.2Ti0.2)B2-SiC Borothermal & Synthesis optimization and Zhang et al.
Powder Hexagonal
(Hf0.2Mo0.2Ta0.2Nb0.2Ti0.2)B2-SiC borocarbothermal reduction mechanical properties (2020) [749]
Experimental verification of
Borocarbothermal reduction Backman et al.
(Hf0.2Zr0.2Ti0.2Ta0.2Nb0.2)B2 Pellet computationally predicted
& spark plasma sintering (2020) [264]
oxidation
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Table A4 (continued )
Ceramic Composition Sample Crystal Structure Synthesis Method Investigated Properties Reference
Shape

(Hf,Zr,Ti,Ta,Nb)B2 Pellet Hexagonal Spark plasma sintering Mechanical properties Feng et al.
(2021) [764]
(Hf0.2Zr0.2Ta0.2Cr0.2Ti0.2)B2 Pellet Hexagonal Borocarbothermal & spark Mechanical properties Zhang et al.
plasma sintering (2021) [763]
(Ti0.2Zr0.2Hf0.2Nb0.2Ta0.2)B2 Thermal and elastic properties by machine learning Dai et al. (2021)
[270]
(Y0.2Nd0.2Sm0.2Gd0.2Tb0.2)B4 Pellet Tetragonal Ball-mill & reactive spark Mechanical properties Qin et al. (2021)
plasma sintering [748]
(V0.2Cr0.2Nb0.2Mo0.2Ta0.2)3B4 Orthorhombic Ball mill & reactive spark Qin et al. (2021)
Pellet Mechanical properties
(V0.2Cr0.2Nb0.2Ta0.2W0.2)3B4 (mainly) plasma sintering [750]
(Y0.2Nd0.2Sm0.2Gd0.2Yb0.2)B6
(Y0.2La0.2Pr0.2Dy0.2Yb0.2)B6
(La0.2Nd0.2Sm0.2Gd0.2Yb0.2)B6 Ball mill & reactive spark Qin et al. (2021)
Pellet Cubic Mechanical properties
(Y0.2La0.2Nd0.2Sm0.2Gd0.2)B6 plasma sintering [751]
(Y0.2La0.2Nd0.2Sm0.2Tb0.2)B6
(La0.2Pr0.2Nd0.2Sm0.2Tb0.2)B6
Borocarbothermal reduction Densification and thermal Monteverde et al.
(Ti,Ta,Nb,Zr,Hf)B2 Pellet Hexagonal
& spark plasma sintering properties (2021) [752]
(Hf0.2Nb0.2Ta0.2Mo0.2Ti0.2)B2
Self-propagating & spark Barbarossa et al.
(Hf0.2Zr0.2Ta0.2Mo0.2Ti0.2)B2 Bulk Hexagonal Mechanical properties
plasma sintering (2021) [753]
(Hf0.2Zr0.2Nb0.2Mo0.2Ti0.2)B2
Ball mill & reactive spark Long et al.
FeCoNiAlCrBx Bulk FCC + BCC Mechanical properties
plasma sintering (2021) [754]
1.(Y0.2Nd0.2Sm0.2Eu0.2Er0.2)B6/
(Y0.2Nd0.2Sm0.2Eu0.2Er0.2)B4
2.(Y0.2Nd0.2Sm0.2Er0.2Yb0.2)B6/
(Y0.2Nd0.2Sm0.2Er0.2Yb0.2)B4, 3.
(Y0.2Nd0.2Eu0.2Er0.2Yb0.2)B6/ Cubic + Borocarbothermal reduction, Zhang et al.
Powder Electromagnetic wave absorption
(Y0.2Nd0.2Eu0.2Er0.2Yb0.2)B4, Tetragonal calcination & grinding (2021) [755]
4.(Nd0.2Sm0.2Eu0.2Er0.2Yb0.2)B6/
(Nd0.2Sm0.2Eu0.2Er0.2Yb0.2)B4
5.(Y0.2 Sm0.2Eu0.2Er0.2Yb0.2)B6/
(Y0.2Sm0.2Eu0.2Er0.2Yb0.2)B4
Iwan et al.
(Hf0.2Ti0.2Zr0.2Ta0.2Mo0.2)B2 Powder Hexagonal Ball mill Mechanical and thermal properties
(2021) [756]
Ball mill & oscillatory Li et al. (2021)
(Zr0.2Ta0.2Nb0.2Hf0.2Mo0.2)B2 Pellet Hexagonal Mechanical and thermal properties
pressure sintering [757]
Ball mill & microwave plasma Storr et al.
(Ta,Mo,Hf,Zr,Ti)B2 Disk Hexagonal Optimizing rapid synthesis
sintering (2021) [758]
(Hf0.2Zr0.2Ti0.2Ta0.2V0.2)B2
(Hf0.2Zr0.2Ti0.2Ta0.2Cr0.2)B2
Ball mill, borocarbothermal
(Hf0.2Zr0.2Ti0.2Ta0.2Nb0.2)B2 Feng et al.
Pellet Hexagonal reduction & spark plasma Mechanical properties
(Hf0.2Zr0.2Ti0.2Ta0.2Mo0.2)B2 (2021) [759]
sintering
(Hf0.2Zr0.2Ti0.2Ta0.2W0.2)B2
(Hf0.2Zr0.2Ti0.2Mo0.2W0.2)B2
(Ti0.2Zr0.2Hf0.2Nb0.2Ta0.2)B2
Ball mill & reactive spark Segregation, precipitation and Wang et al.
(Zr0.2Hf0.2Nb0.2Ta0.2W0.2)B2 Pellet Hexagonal
plasma sintering mechanical properties (2021) [760]
(Zr0.225Hf0.225Nb0.225Mo0.225W0.1)B2
(Hf0.2Mo0.2Ta0.2Nb0.2Ti0.2)B2 Self-propagating, ball mill & Densification behavior by adding Barbarossa et al.
Disk Multi-phases
(Hf0.2Mo0.2Ta0.2Zr0.2Ti0.2)B2 spark plasma sintering graphite (2021) [761]
(Ce0.2Y0.2Sm0.2Er0.2Yb0.2)B6
(Ce0.2Eu0.2Sm0.2Er0.2Yb0.2)B6
Borocarbothermal reduction, Zhang et al.
(Ce0.2Y0.2Eu0.2Er0.2Yb0.2)B6 Powder Cubic Electromagnetic absorption
heating & grinding (2021) [762]
(Ce0.2Y0.2Sm0.2Eu0.2Yb0.2)B6
(Nd0.2Y0.2Sm0.2Eu0.2Yb0.2)B6

Table A5
Summary of publications about high-entropy hydrides in chronological order. Information before and after→ correspond to alloy and hydride, respectively.
Ceramic Composition Sample Crystal Structure Synthesis Method Investigated Reference
Shape Properties

Ingot → C14 Laves → Hydrogen Kao et al. (2010)

CoFeMnTixVyZrz-H Arc melting & hydrogenation
Powder C14 Laves storage [63]
Layer → Laser engineered net shaping & Hydrogen Kunce et al. (2013)
ZrTiVCrFeNi-H C14 Laves + HCP → C14 Laves
Powder hydrogenation storage [213]
layer → Laser engineered net shaping & Hydrogen Kunce et al. (2014)
TiZrNbMoV-H BCC + Orthorhombic → BCC
Powder hydrogenation storage [218]
Ingot → BCC + C14 (x = 0, 0.5) or FCC (x = Hydrogen Yang et al. (2016)
(VFe)60(TiCrCo) 40-xZrx-H (0 ≤ x ≤ 2) Arc melting & hydrogenation
Powder 1, 2) → Not reported storage [220]
Ingot → Hydrogen Sahlberg et al.
TiVZrNbHf-H BCC → BCT Arc melting & hydrogenation
Powder storage (2016) [219]
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Table A5 (continued )
Ceramic Composition Sample Crystal Structure Synthesis Method Investigated Reference
Shape Properties

LaNiFeVMn-H Layer → Hexagonal + Tetragonal or Laser metal deposition & Hydrogen Kunce et al. (2017)
Powder Hexagonal + FCC → Not reported hydrogenation storage [221]
MgZrTiFe0.5Co0.5Ni0.5-H Powder → BCC → FCC Ball mill & hydrogenation Hydrogen Zepon et al. (2018)
Powder storage [215]
LiBH4NaBH4KBH4Mg(BH4)2Ca Powder → Multi-phases Ball mill & hydrogenation Hydrogen Dematteis et al.
(BH4)2 Powder storage (2018) [216]
HfNbTiVZr-H Ingot → BCC → BCT Arc melting & hydrogenation Hydrogen Karlsson et al.
Powder storage (2018) [214]
TiZrNbHfTa-H Ingot → BCC → FCC Arc melting & hydrogenation Hydrogen Zlotea et al. (2019)
Powder storage [222]
Ti-V-Zr-Nb-Ta-H Ingot → BCC → FCC Arc melting & hydrogenation Hydrogen Nygård et al.
Powder storage (2019) [224]
LaNi4.8Fe0.3Mn0.1LaNi4.6Al0.2Mn0.2-
H
LaNi4.6Al0.2Mn0.2-H
Ingot → Hydrogen Kazakov et al.
LaNi4.8Al0.2-H CaCu5-type → Not reported Arc melting & hydrogenation
Powder storage (2019) [777]
La0.9Ce0.1Ni5-H
La0.7Ce0.3Ni5-H
MnNi4.15Fe0.85-H
TiVNb-H
TiVCrMo-H
TiZrNbHf-H
Ingot → Hydrogen Nygård et al.
TiVNbM-H (M = Cr, Zr, Mo, Hf, Ta) BCC → FCC Arc melting & hydrogenation
Powder storage (2019) [223]
TiVZrNbHf-H
TiVCrNbMo-H
TiVCrNbTa-H
Ingot → Intermetallics + BCC → Not Hydrogen Spaliviero et al.
TiV0.6Cr0.3Zr0.3NbMo-H Arc melting & hydrogenation
Powder reported storage (2019) [778]
Ingot → Hydrogen Hu et al. (2019)
TiZrHfScMo-H BCC → Not reported Arc melting & hydrogenation
Powder storage [225]
Ingot → Hydrogen Montero et al.
Ti0.30V0.25Zr0.10Nb0.25Ta0.10-H BCC → FCC Arc melting & hydrogenation
Powder storage (2020) [226]
I. Ti0.2Zr0.2Hf0.2Nb0.4-H I. BCC → FCC
II. Ti0.2Zr0.2Hf0.2Mo0.1Nb0.3-H II. BCC → FCC
Ingot → Hydrogen Shen et al. (2020)
III. Ti0.2Zr0.2Hf0.2Mo0.2Nb0.2-H III. BCC → FCC Arc melting & hydrogenation
Powder storage [217]
IV. Ti0.2Zr0.2Hf0.2Mo0.3Nb0.1-H IV. BCC → BCT
V. Ti0.2Zr0.2Hf0.2Mo0.4-H V. BCC → BCT
Ingot → Hydrogen Zhang et al. (2020)
TiZrNbTa-H BCC → Multi-hydride phases Arc melting & hydrogenation
Powder storage [789]
Powder → Hydrogen Dewangan et al.
AlCrFeMnNiW-H BCC + FCC → BCC + FCC Ball mill & hydrogenation
Powder storage (2020) [227]
I. MgVCr-H I. BCC → Multi-hydride phases
Disk → Ball mill, reactive milling, high- Hydrogen Marco et al. (2020)
II. BCC + Amorphous → Multi-
II. MgVTiCrFe-H Powder pressure torsion & hydrogenation storage [299]
hydride phases
Disk → Hydrogen Edalati et al. (2020)
TiZrCrMnFeNiH6 C14 Laves + B2 cubic → C14 Laves Arc melting & hydrogenation
Powder storage [271]
Disk → Hydrogen Floriano et al.
TiZrNbFeNi-H C14 Laves + B2 cubic → C14 Laves Arc melting & hydrogenation
Powder storage (2020) [278]
Powder → Hydrogen Strozi et al. (2021)
Mg-V-Al-Cr-Ni-H BCC → BCC Reactive ball mill
Powder storage [788]
Zhang et al. (2021)
TiZrVMoNb-H Hydrogen desorption investigation by DFT calculations
[235]
Hu et al. (2021)
TiZrVMoNb-H Hydrogen storage investigation using DFT calculations
[236]
Powder → Hydrogen Strozi et al. (2021)
Mg12Al11Ti33Mn11Nb33-H BCC → BCC Ball mill & hydrogenation
Powder storage [779]
Pellet → Hydrogen Sleiman et al.
TiVZrHfNb-H BCC → BCT Arc melting & hydrogenation
Powder storage (2021) [780]
Ingot → Hydrogen Montero et al.
Al0.10Ti0.30V0.25Zr0.10Nb0.25-H BCC → BCT Arc melting & hydrogenation
Powder storage (2021) [781]
Powder → Hydrogen Cardoso et al.
MgAlTiFeNi-H BCC → BCC + FCC + Mg2FeH6-type Ball mill & reactive ball mill
Powder storage (2021) [782]
Ingot → C14 Laves + BCC → C14 Laves + Hydrogen Floriano et al.
TiZrNbCrFe-H Arc melting & hydrogenation
Powder FCC storage (2021) [783]
Powder → Hydrogen Montero et al.
Mg0.10Ti0.30V0.25Zr0.10Nb0.25-H BCC → FCC Ball mill & reactive ball mill
Powder storage (2021) [784]
V35Ti30Cr25Fe10-H
V35Ti30Cr25Mn10-H Pellet → Hydrogen Liu et al. (2021)
BCC → BCT + FCC Arc melting & hydrogenation
V30Ti30Cr25Fe10Nb5-H Powder storage [785]
V35Ti30Cr25Fe5Mn5-H
Ingot → Hydrogen Park et al. (2021)
TiZrVNbCr-H BCC + FCC → FCC + FCC Arc melting & hydrogenation
Powder storage [786]
Hu et al. (2021)
TiZrHfMoNb-H Hydrogen storage properties and hydrogen effect on mechanical properties using DFT calculations
[237]
TiVNb-H BCC/HCP → FCC/BCT Arc melting & hydrogenation
(continued on next page)

53
S. Akrami et al. Materials Science & Engineering R 146 (2021) 100644

Table A5 (continued )
Ceramic Composition Sample Crystal Structure Synthesis Method Investigated Reference
Shape Properties

TiVZr0.5Nb-H
TiVZrNb-H
Ingot → Vibrational Ek et al. (2021)
TiVZrNbHf0.5-H
Powder properties [787]
TiVZrNbHf-H
TiZrHf-H

Table A6
Summary of publications about other high-entropy ceramics in chronological order.
Ceramic Composition Sample Crystal Structure Synthesis Method Investigated Properties Reference
Shape

(AlCrTaTiZr)NxCy Film FCC Co-sputtering Mechanical properties Chang et al.

(2011) [60]
(Ti,Ta,Nb)CxN1-x Cylindrical Cubic Ball mill & sintering Hardness as cermet Obra et al.
shape (2017) [76]
Cu5SnMgGeZnS9 Designing by a data-driven
Ball mill & spark plasma Zhang et al.
Bulk Tetragonal model and using them as
Cu3SnMgInZnS7 sintering (2018) [69]
thermoelectric materials
Microstructure and mechanical Le et al. (2018)
CoCrFeMnNi-ON Film FCC + Amorphous DC magnetron sputtering
properties [74]
Wang et al.
Lix(Co0.2Cu0.2Mg0.2Ni0.2Zn0.2)OFx Powder Rock-salt Ball mill Li ion conductivity
(2019) [96]
Structural features and thermal Zhao et al.
(La0.2Ce0.2Nd0.2Sm0.2Eu0.2)PO4 Powder Monoclinic Co-precipitation
properties (2019) [73]
Ball mill & spark plasma Thermal conductivity, hardness Gild et al.
(Mo0.2Nb0.2Ta0.2Ti0.2W0.2)Si2 Disk C40 hexagonal
sintering and elastic modulus (2019) [64]
Zhang et al.
High-Entropy Ceramics Review paper on high-entropy ceramics
(2019) [41]
Ball mill & reactive spark Qin et al.
(Ti0.2Zr0.2Nb0.2Mo0.2W0.2)Si2 Bulk HCP Mechanical properties
plasma sintering (2019) [65]
Ball mill & reactive spark Microstructure and mechanical Liu et al.
(Mo0.2W0.2Cr0.2Ta0.2Nb0.2)Si2 Bulk C40 hexagonal
plasma sintering properties (2020) [67]
Ball mill & spark plasma Microstructure and mechanical Qin (et al.
(TiZrNbMoW)Si2 Bulk HCP
sintering properties 2020) [68]
Zhao et al.
Co-Cr-Fe-Mn-Ni-P Nano-sheet Cubic Eutectic synthesis Electrocatalytic water splitting
(2020) [72]
Wen et al.
(Mo0.25Nb0.25Ta0.25V0.25)(Al0.5Si0.5)2 Powder C40 hexagonal Solid-state reaction Optimizing synthesis
(2020) [66]
Nano- Chen et al.
CeNdCaSrBaF12 Cubic Co-precipitation Laser application
powder (2020) [70]
K(MgMnFeCoNi)F3
K(MgMnCoNiZn)F3 Hydrothermal method with Wang et al.
Powder Perovskite Electrocatalysis
K(MnFeCoNiZn)F3 mechano-chemistry (2020) [71]
K(MgCoNiCuZn)F3
Wright et al.
High-Entropy Ceramics Review on compositionally complex ceramics
(2020) [40]
Oses et al.
High-Entropy Ceramics Review paper on high-entropy ceramics
(2020) [129]
Cubic (carbide) +
Ball mill & spark plasma Mechanical and thermal Qin et al.
(Ti-Zr-Nb-Hf-Ta-W)C + (Ti-Zr-Nb-Hf-Ta-W)B2 Pellet Hexagonal
sintering properties (2020) [837]
(boride)
(Ta0.2Nb0.2Zr0.2Hf0.2W0.2)BCN
Guan et al.
(Ta0.2Nb0.2Zr0.2Hf0.2Ti0.2)BCN Powder FCC Ball mill Thermal stability
(2020) [75]
(Ta0.2Nb0.2Zr0.2Ti0.2W0.2)BCN
Li1.3 Mn3+0.4Ti0.3O1.7F0.3
Lun et al.
Li1.3 Mn2+0.2 Mn3+0.2Ti0.1Nb0.2O1.7F0.3 Powder Rock-salt Solid-state reaction Li-ion batteries
(2021) [438]
Li1.3Mn2+0.1Co2+0.1Mn3+0.1Cr3+0.1Ti0.1Nb0.2O1.7F0.3
Ball milling & carbothermal Ma et al.
(Hf,Zr,Ta,Nb,Ti)(C,N) Powder Cubic Synthesis possibility
reduction nitridation (2021) [832]
Ball mill & spark plasma Peng et al.
(Ta0.2Hf0.2Zr0.2Ti0.2Nb0.2)C0.8N0.2 Pellet FCC Ablation resistance
sintering (2021) [833]
(Ti0.33Zr0.33Hf0.33)(C0.5N0.5)
Ball mill & spark plasma Sintering behavior and Zhang et al.
(Ti0.25Zr0.25Hf0.25Nb0.25)(C0.5N0.5) Bulk FCC (mainly)
sintering toughness (2021) [834]
(Ti0.2Zr0.2Hf0.2Nb0.2Ta0.2)(C0.5N0.5)
High pressure torsion + Photocatalytic hydrogen Edalati et al.
TiZrHfNbTaO6N3 Powder FCC + Monoclinic
Oxidation + nitriding production from water splitting (2021) [298]
Monoclinic + Qiao et al.
CoFeNiMnMo-PO4 Bulk Fly-through method Catalysis
Cubic (2021) [829]
(CrMoTa)Si2 Electron beam evaporation Design by CALPHAD and Vyatskikh et al.
Film C40 hexagonal
(CrMoTaVNb)Si2 & heat treatment synthesis (2021) [238]
Chen et al.
(Mo0.25Nb0.25Ta0.25V0.25) (Al0.5Si0.5)2 Effect of lattice distortion on thermodynamic properties by DFT calculations
(2021) [239]
(continued on next page)

54
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Table A6 (continued )
Ceramic Composition Sample Crystal Structure Synthesis Method Investigated Properties Reference
Shape

(CuNiFeZn)F2
(CuNiFeCoZn)F2
Sukkurji et al.
(CuNiFeCoMn)F2 Powder Rutile-type Ball mill Electrocatalysis
(2021) [825]
(CuNiFeCoZnMn)F2
(CuNiFeCoZnMnMg)F2
Borocarbothermal
(Ti0.2Zr0.2Hf0.2Nb0.2Ta0.2)B2 + Cubic carbide + Microstructure and mechanical Luo et al.
Pellet reduction & spark plasma
(Ti0.2Zr0.2Hf0.2Nb0.2Ta0.2)C Hexagonal boride propertied (2021) [836]
sintering
Edalati et al.
High-Entropy Materials Review paper on high-entropy materials synthesized by high-pressure torsion
(2021) [296]

References [49] C.Y. Hsu, J.W. Yeh, S.K. Chen, T.T. Shun, Metall. Mater. Trans. A 35 (2004)
1465–1469.
[50] P.K. Huang, J.W. Yeh, T.T. Shun, S.K. Chen, Adv. Eng. Mater. 6 (2004) 74–78.
[1] J.W. Yeh, S.K. Chen, S.J. Lin, J.Y. Gan, T.S. Chin, T.T. Shun, C.H. Tsau, S.
[51] B.S. Murty, J.W. Yeh, S. Ranganathan, P. Bhattacharjee, High-Entropy Alloys,
Y. Chang, Adv. Eng. Mater. 6 (2004) 299–303.
second ed., Elsevier, 2019.
[2] B. Cantor, I. Chang, P. Knight, A. Vincent, Mater. Sci. Eng. A 375 (2004) 213–218.
[52] B. Cantor, K. Kim, P.J. Warren, J. Metastable Nanocryst. Mater. 386-388 (2002)
[3] Y. Jien-Wei, Ann. Chim. Sci. Mat. 31 (2006) 633–648.
27–32.
[4] Y. Zhou, Y. Zhang, Y. Wang, G. Chen, Appl. Phys. Lett. 90 (2007), 181904.
[53] B. Cantor, Entropy 16 (2014) 4749–4768.
[5] X. Wang, Y. Zhang, Y. Qiao, G. Chen, Intermetallics 15 (2007) 357–362.
[54] T.K. Chen, M.S. Wong, T.T. Shun, J.W. Yeh, Surf. Coat. Technol. 200 (2005)
[6] Y. Zhang, Y.J. Zhou, J.P. Lin, G.L. Chen, P.K. Liaw, Adv. Eng. Mater. 10 (2008)
1361–1365.
534–538.
[55] Y. Zhang, High-Entropy Materials, first ed., Springer, 2019.
[7] C. Li, J. Li, M. Zhao, Q. Jiang, J. Alloys. Compd. 475 (2009) 752–757.
[56] T.K. Chen, M.S. Wong, Thin Solid Films 516 (2007) 141–146.
[8] O. Senkov, G. Wilks, D. Miracle, C. Chuang, P. Liaw, Intermetallics 18 (2010)
[57] T.K. Chen, M.S. Wong, Surf. Coat. Technol. 203 (2008) 495–500.
1758–1765.
[58] C.M. Rost, E. Sachet, T. Borman, A. Moballegh, E.C. Dickey, D. Hou, J.L. Jones,
[9] S. Singh, N. Wanderka, B. Murty, U. Glatzel, J. Banhart, Acta Mater. 59 (2011)
S. Curtarolo, J.P. Maria, Nat. Commun. 6 (2015) 8485.
182–190.
[59] M. Braic, V. Braic, M. Balaceanu, C. Zoita, A. Vladescu, E. Grigore, Surf. Coat.
[10] O.N. Senkov, G. Wilks, J. Scott, D.B. Miracle, Intermetallics 19 (2011) 698–706.
Technol. 204 (2010) 2010–2014.
[11] C.M. Lin, H.L. Tsai, Intermetallics 19 (2011) 288–294.
[60] S.Y. Chang, S.Y. Lin, Y.C. Huang, Thin Solid Films 519 (2011) 4865–4869.
[12] M.H. Chuang, M.H. Tsai, W.R. Wang, S.J. Lin, J.W. Yeh, Acta Mater. 59 (2011)
[61] J. Gild, Y. Zhang, T. Harrington, S. Jiang, T. Hu, M.C. Quinn, W.M. Mellor,
6308–6317.
N. Zhou, K. Vecchio, J. Luo, Sci. Rep. 6 (2016) 37946.
[13] G. Sheng, C.T. Liu, Prog. Nat. Sci. 21 (2011) 433–446.
[62] S.W. Cho, H. Enoki, E. Akiba, J. Alloys. Compd. 307 (2000) 304–310.
[14] S. Guo, C. Ng, J. Lu, C. Liu, J. Aappl. Phys. 109 (2011), 103505.
[63] Y.F. Kao, S.K. Chen, J.H. Sheu, J.T. Lin, W.E. Lin, J.W. Yeh, S.J. Lin, T.H. Liou, C.
[15] X. Yang, Y. Zhang, P. Liaw, Procedia Eng. 36 (2012) 292–298.
W. Wang, Int. J. Hydrogen Energy 35 (2010) 9046–9059.
[16] X. Yang, Y. Zhang, Mater. Chem. Phys. 132 (2012) 233–238.
[64] J. Gild, J. Braun, K. Kaufmann, E. Marin, T. Harrington, P. Hopkins, K. Vecchio,
[17] Y. Zhang, X. Yang, P. Liaw, JOM 64 (2012) 830–838.
J. Luo, J. Materiomics 5 (2019) 337–343.
[18] M.A. Hemphill, T. Yuan, G. Wang, J. Yeh, C. Tsai, A. Chuang, P. Liaw, Acta Mater.
[65] Y. Qin, J.X. Liu, F. Li, X. Wei, H. Wu, G.J. Zhang, J. Adv. Ceram. 8 (2019)
60 (2012) 5723–5734.
148–152.
[19] W.R. Wang, W.L. Wang, S.C. Wang, Y.C. Tsai, C.H. Lai, J.W. Yeh, Intermetallics
[66] T. Wen, H. Liu, B. Ye, D. Liu, Y. Chu, Sci. China Mater. 63 (2020) 300–306.
26 (2012) 44–51.
[67] D. Liu, Y. Huang, L. Liu, L. Zhang, Mater. Lett. 268 (2020), 127629.
[20] Y. Zhang, T. Zuo, Y. Cheng, P.K. Liaw, Sci. Rep. 3 (2013) 1455.
[68] Y. Qin, J.C. Wang, J.X. Liu, X.F. Wei, F. Li, G.J. Zhang, C. Jing, J. Zhao, H. Wu,
[21] F. Otto, Y. Yang, H. Bei, E.P. George, Acta Mater. 61 (2013) 2628–2638.
J. Eur. Ceram. Soc. 40 (2020) 2752–2759.
[22] J.W. Yeh, JOM 65 (2013) 1759–1771.
[69] R.Z. Zhang, F. Gucci, H. Zhu, K. Chen, M.J. Reece, Inorg. Chem. 57 (2018)
[23] M.H. Tsai, J.W. Yeh, Mater. Res. Lett. 2 (2014) 107–123.
13027–13033.
[24] Y. Zhang, T.T. Zuo, Z. Tang, M.C. Gao, K.A. Dahmen, P.K. Liaw, Z.P. Lu, Prog.
[70] X. Chen, Y. Wu, J. Am. Ceram. Soc. 103 (2020) 750–756.
Mater. Sci. 61 (2014) 1–93.
[71] T. Wang, H. Chen, Z. Yang, J. Liang, S. Dai, J. Am. Chem. Soc. 142 (2020)
[25] D.B. Miracle, J.D. Miller, O.N. Senkov, C. Woodward, M.D. Uchic, J. Tiley,
4550–4554.
Entropy 16 (2014) 494–525.
[72] X. Zhao, Z. Xue, W. Chen, Y. Wang, T. Mu, ChemSusChem 13 (2020) 2038–2042.
[26] Y. Lu, Y. Dong, S. Guo, L. Jiang, H. Kang, T. Wang, B. Wen, Z. Wang, J. Jie, Z. Cao,
[73] Z. Zhao, H. Chen, H. Xiang, F.-Z. Dai, X. Wang, Z. Peng, Y. Zhou, J. Mater. Sci.
Sci. Rep. 4 (2014) 6200.
Technol. 35 (2019) 2892–2896.
[27] Y. Ye, Q. Wang, J. Lu, C. Liu, Y. Yang, Mater. Today 19 (2016) 349–362.
[74] D.D. Le, S.-K. Hong, T.S. Ngo, J. Lee, Y.C. Park, S.I. Hong, Y.-S. Na, Met. Mater.
[28] M.C. Gao, J.W. Yeh, P.K. Liaw, Y. Zhang, High-Entropy Alloys, first ed., Springer
Int. 24 (2018) 1285–1292.
International Publishing, Switzerland, 2016.
[75] J. Guan, D. Li, Z. Yang, B. Wang, D. Cai, X. Duan, P. He, D. Jia, Y. Zhou, Ceram.
[29] E. Pickering, N. Jones, Int. Mater. Rev. 61 (2016) 183–202.
Int. 46 (2020) 26581–26589.
[30] D.B. Miracle, O.N. Senkov, Acta Mater. 122 (2017) 448–511.
[76] A. De la Obra, M. Avilés, Y. Torres, E. Chicardi, F. Gotor, Int. J. Refract. Metals
[31] C. Toher, C. Oses, D. Hicks, S. Curtarolo, Npj Comput. Mater. 5 (2019) 69.
Hard Mater. 63 (2017) 17–25.
[32] A. Sarkar, Q. Wang, A. Schiele, M.R. Chellali, S.S. Bhattacharya, D. Wang,
[77] J. Zhang, J. Yan, S. Calder, Q. Zheng, M.A. McGuire, D.L. Abernathy, Y. Ren, S.
T. Brezesinski, H. Hahn, L. Velasco, B. Breitung, Adv. Mater. 31 (2019), 1806236.
H. Lapidus, K. Page, H. Zheng, Chem. Mater. 31 (2019) 3705–3711.
[33] S.J. McCormack, A. Navrotsky, Acta Mater. 202 (2021) 1–21.
[78] Z. Zhao, H. Chen, H. Xiang, F.-Z. Dai, X. Wang, W. Xu, K. Sun, Z. Peng, Y. Zhou,
[34] J.W. Yeh, Y.L. Chen, S.J. Lin, S.K. Chen, Mater. Sci. Forum 560 (2007) 1–9.
J. Mater. Sci. Technol. 39 (2020) 167–172.
[35] A. Sarkar, B. Breitung, H. Hahn, Scr. Mater. 187 (2020) 43–48.
[79] R. Witte, A. Sarkar, R. Kruk, B. Eggert, R.A. Brand, H. Wende, H. Hahn, Phys. Rev.
[36] J.W. Yeh, S.J. Lin, T.S. Chin, J.Y. Gan, S.K. Chen, T.T. Shun, C.H. Tsau, S.-
B Condens. Matter Mater. Phys. 3 (2019), 034406.
Y. Chou, Metall. Mater. Trans. A 35 (2004) 2533–2536.
[80] F. Okejiri, Z. Zhang, J. Liu, M. Liu, S. Yang, S. Dai, ChemSusChem 13 (2020)
[37] B.L. Musicó, D. Gilbert, T.Z. Ward, K. Page, E. George, J. Yan, D. Mandrus,
111–115.
V. Keppens, APL Mater. 8 (2020), 040912.
[81] J.C. Rendón-Angeles, Z. Matamoros-Veloza, K.L. Montoya-Cisneros, J. López
[38] Y. Zhang, T. Zuo, Y. Cheng, P.K. Liaw, Sci. Rep. 3 (2013) 1455.
Cuevas, K. Yanagisawa, in: L. Pan, G. Zhu (Eds.), Perovskite Materials: Synthesis,
[39] A.J. Wright, Q. Wang, C. Huang, A. Nieto, R. Chen, J. Luo, J. Eur. Ceram. Soc. 40
Characterisation, Properties, and Applications, IntechOpen, 2016, pp. 27–82.
(2020) 2120–2129.
[82] D. Wang, Z. Liu, S. Du, Y. Zhang, H. Li, Z. Xiao, W. Chen, R. Chen, Y. Wang,
[40] A.J. Wright, J. Luo, J. Mater. Sci. 55 (2020) 9812–9827.
Y. Zou, J. Mater. Chem. A Mater. Energy Sustain. 7 (2019) 24211–24216.
[41] R.Z. Zhang, M.J. Reece, J. Mater. Chem. A 7 (2019) 22148–22162.
[83] F. Li, L. Zhou, J.X. Liu, Y. Liang, G.J. Zhang, J. Adv. Ceram. 8 (2019) 576–582.
[42] W. Zhang, P.K. Liaw, Y. Zhang, Sci. China Mater. 61 (2018) 2–22.
[84] E. Lewin, J. Appl. Phys. 127 (2020), 160901.
[43] Q. He, Z. Ding, Y. Ye, Y. Yang, JOM 69 (2017) 2092–2098.
[85] S. Jiang, L. Shao, T.W. Fan, J.M. Duan, X.T. Chen, B.Y. Tang, Ceram. Int. 46
[44] C.S. Smith, Four Outstanding Researches in Metallurgical History, first ed.,
(2020) 15104–15112.
American Society for Testing and Materials, USA, 1963.
[86] J. Gild, Y. Zhang, T. Harrington, S. Jiang, T. Hu, M.C. Quinn, W.M. Mellor,
[45] A.L. Greer, Nature 366 (1993) 303–304.
N. Zhou, K. Vecchio, J. Luo, Sci. Rep. 6 (2016) 37946.
[46] B. Cantor, F. Audebert, M. Galano, K. Kim, I. Stone, P.J. Warren, J. Metastable
[87] Z. Rak, C. Rost, M. Lim, P. Sarker, C. Toher, S. Curtarolo, J.-P. Maria, D. Brenner,
Nanocryst. Mater. 24-25 (2005) 1–6.
J. Appl. Phys. 120 (2016), 095105.
[47] B. Cantor, Ann. Chem.-Sci. Mater. 32 (2007) 245–256.
[88] D. Bérardan, S. Franger, D. Dragoe, A.K. Meena, N. Dragoe, Phys. Status Solidi
[48] T. Chen, T. Shun, J. Yeh, M. Wong, Surf. Coat. Technol. 188 (2004) 193–200.
RRL 10 (2016) 328–333.

55
S. Akrami et al.
[89] D. Berardan, A. Meena, S. Franger, C. Herrero, N. Dragoe, J. Alloys. Compd. 704
(2017) 693–700.
[90] C.M. Rost, Z. Rak, D.W. Brenner, J.P. Maria, J. Am. Ceram. Soc. 100 (2017)
2732–2738.
[91] J. Chen, W. Liu, J. Liu, X. Zhang, M. Yuan, Y. Zhao, J. Yan, M. Hou, J. Yan,
M. Kunz, J. Phys. Chem. C 123 (2019) 17735–17744.
[92] N. Osenciat, D. Bérardan, D. Dragoe, B. Leridon, S. Holé, A.K. Meena, S. Franger,
N. Dragoe, J. Am. Ceram. Soc. 102 (2019) 6156–6162.
[93] A.D. Dupuy, X. Wang, J.M. Schoenung, Mater. Res. Lett. 7 (2019) 60–67.
[94] H. Chen, W. Lin, Z. Zhang, K. Jie, D.R. Mullins, X. Sang, S.-Z. Yang, C.J. Jafta, C.
A. Bridges, X. Hu, ACS Mater. Lett. 1 (2019) 83–88.
[95] M. Balcerzak, K. Kawamura, R. Bobrowski, P. Rutkowski, T. Brylewski, J. Korean
Inst. Electr. Electron. Mater. Eng. 48 (2019) 7105–7113.
[96] Q. Wang, A. Sarkar, D. Wang, L. Velasco, R. Azmi, S.S. Bhattacharya, T. Bergfeldt,
A. Düvel, P. Heitjans, T. Brezesinski, Energy Environ. Sci. 12 (2019) 2433–2442.
[97] Y. Zheng, Y. Yi, M. Fan, H. Liu, X. Li, R. Zhang, M. Li, Z.-A. Qiao, Energy Storage
Mater. 23 (2019) 678–683.
[98] M.P. Jimenez-Segura, T. Takayama, D. Bérardan, A. Hoser, M. Reehuis, H. Takagi,
N. Dragoe, Appl. Phys. Lett. 114 (2019), 122401.
[99] Z. Grzesik, G. Smoła, M. Stygar, J. Dąbrowa, M. Zajusz, K. Mroczka,
M. Danielewski, J. Eur. Ceram. Soc. 39 (2019) 4292–4298.
[100] W. Hong, F. Chen, Q. Shen, Y.H. Han, W.G. Fahrenholtz, L. Zhang, J. Am. Ceram.
Soc. 102 (2019) 2228–2237.
[101] Q. Wang, A. Sarkar, Z. Li, Y. Lu, L. Velasco, S.S. Bhattacharya, T. Brezesinski,
H. Hahn, B. Breitung, Electrochem. commun. 100 (2019) 121–125.
[102] M.R. Chellali, A. Sarkar, S.H. Nandam, S.S. Bhattacharya, B. Breitung, H. Hahn,
L. Velasco, Scr. Mater. 166 (2019) 58–63.
[103] A. Sarkar, R. Djenadic, N.J. Usharani, K.P. Sanghvi, V.S. Chakravadhanula, A.
S. Gandhi, H. Hahn, S.S. Bhattacharya, J. Eur. Ceram. Soc. 37 (2017) 747–754.
[104] A. Sarkar, L. Velasco, D. Wang, Q. Wang, G. Talasila, L. de Biasi, C. Kübel,
T. Brezesinski, S.S. Bhattacharya, H. Hahn, B. Breitung, Nat. Commun. 9 (2018)
3400.
[105] N.J. Usharani, A. Bhandarkar, S. Subramanian, S.S. Bhattacharya, Acta Mater.
200 (2020) 526–536.
[106] A. Kumar, G. Sharma, A. Aftab, M.I. Ahmad, J. Eur. Ceram. Soc. 40 (2020)
3358–3362.
[107] D. Liu, X. Peng, J. Liu, L. Chen, Y. Yang, L. An, J. Eur. Ceram. Soc. 40 (2020)
2504–2508.
[108] B. Yoon, V. Avila, R. Raj, L.M. Jesus, Scr. Mater. 181 (2020) 48–52.
[109] M. Biesuz, L. Spiridigliozzi, G. Dell’Agli, M. Bortolotti, V.M. Sglavo, J. Mater. Sci.
53 (2018) 8074–8085.
[110] A. Mao, H.Z. Xiang, Z.G. Zhang, K. Kuramoto, H. Yu, S. Ran, J. Magn. Magn.
Mater. 484 (2019) 245–252.
[111] H.Z. Xiang, H.X. Xie, A. Mao, Y.-G. Jia, T.Z. Si, Int. J. Mater. Res. 111 (2020)
246–249.
[112] G.N. Kotsonis, C.M. Rost, D.T. Harris, J.P. Maria, MRS Commun. 8 (2018)
1371–1377.
[113] D. Bérardan, S. Franger, A. Meena, N. Dragoe, J. Mater. Chem. A Mater. Energy
Sustain. 4 (2016) 9536–9541.
[114] P. Ghigna, L. Airoldi, M. Fracchia, D. Callegari, U. Anselmi-Tamburini,
P. D’angelo, N. Pianta, R. Ruffo, G. Cibin, D.O. de Souza, E. Quartarone, ACS
Appl. Mater. Interfaces 12 (2020) 50344–50354.
[115] S. Sivakumar, E. Zwier, P.B. Meisenheimer, J.T. Heron, J. Vis. Exp. 135 (2018)
57746.
[116] P.B. Meisenheimer, L.D. Williams, S.H. Sung, J. Gim, P. Shafer, G.N. Kotsonis, J.-
P. Maria, M. Trassin, R. Hovden, E. Kioupakis, Phys. Rev. B Condens. Matter
Mater. Phys. 3 (2019), 104420.
[117] A.L. Cardoso, C.P. Perdomo, R.H. Kiminami, R.F. Gunnewiek, Mater. Lett. 285
(2021), 129175.
[118] J. Gild, M. Samiee, J.L. Braun, T. Harrington, H. Vega, P.E. Hopkins, K. Vecchio,
J. Luo, J. Eur. Ceram. Soc. 38 (2018) 3578–3584.
[119] J. Dąbrowa, M. Szymczak, M. Zajusz, A. Mikuła, M. Moździerz, K. Berent,
M. Wytrwal-Sarna, A. Bernasik, M. Stygar, K. Świerczek, J. Eur. Ceram. Soc. 40
(2020) 5870–5881.
[120] L. Spiridigliozzi, C. Ferone, R. Cioffi, G. Accardo, D. Frattini, G. Dell’Agli,
Materials 13 (2020) 558.
[121] V. Sachkov, R. Nefedov, I. Amelichkin, IOP Conf. Ser.: Mater. Sci. Eng. 597
(2019), 012005.
[122] C.M. Rost, Entropy-sabilized Oxides: Explorations of a Novel Class of
Multicomponent Materials, PhD Dissertation, North Carolina State University,
2016.
[123] L. Song, M. Rongjun, Asian J. Chem. 19 (2007) 1883.
[124] Y. Liao, L. He, M. Zhao, D. Ye, J. Environ. Chem. Eng. 5 (2017) 5054–5060.
[125] S.M. Pourmortazavi, M. Rahimi-Nasrabadi, M. Aghazadeh, M.R. Ganjali, M.
S. Karimi, P. Norouzi, J. Mol. Struct. 1150 (2017) 411–418.
[126] P. Kim, A. Anderko, A. Navrotsky, R.E. Riman, Minerals 8 (2018) 106.
[127] R. Djenadic, A. Sarkar, O. Clemens, C. Loho, M. Botros, V.S. Chakravadhanula,
C. Kübel, S.S. Bhattacharya, A.S. Gandhi, H. Hahn, Mater. Res. Lett. 5 (2017)
102–109.
[128] A. Sarkar, C. Loho, L. Velasco, T. Thomas, S.S. Bhattacharya, H. Hahn,
R. Djenadic, Dalton Trans. 46 (2017) 12167–12176.
[129] C. Oses, C. Toher, S. Curtarolo, Nat. Rev. Mater. 5 (2020) 295–309.
[130] H. Lehmann, D. Pitzer, G. Pracht, R. Vassen, D. Stöver, J. Am. Ceram. Soc. 86
(2003) 1338–1344.
[131] X. Cao, R. Vassen, D. Stöver, J. Eur. Ceram. Soc. 24 (2004) 1–10.
56
Materials Science & Engineering R 146 (2021) 100644
[132] Q. Xu, W. Pan, J. Wang, C. Wan, L. Qi, H. Miao, K. Mori, T. Torigoe, J. Am. Ceram.
Soc. 89 (2006) 340–342.
[133] A.R. Krause, B.S. Senturk, H.F. Garces, G. Dwivedi, A.L. Ortiz, S. Sampath, N.
P. Padture, J. Am. Ceram. Soc. 97 (2014) 3943–3949.
[134] A.R. Krause, B.S. Senturk, H.F. Garces, G. Dwivedi, A.L. Ortiz, S. Sampath, N.
P. Padture, J. Am. Ceram. Soc. 97 (2014) 3943–3949.
[135] K. Matsui, H. Yoshida, Y. Ikuhara, Int. Mater. Rev. 63 (2018) 375–406.
[136] A. Sarkar, R. Djenadic, D. Wang, C. Hein, R. Kautenburger, O. Clemens, H. Hahn,
J. Eur. Ceram. Soc. 38 (2018) 2318–2327.
[137] R. Witte, A. Sarkar, L. Velasco, R. Kruk, R.A. Brand, B. Eggert, K. Ollefs,
E. Weschke, H. Wende, H. Hahn, J. Appl. Phys. 127 (2020), 185109.
[138] D. Lin, K.W. Kwok, Curr. Appl. Phys. 9 (2009) 1369–1374.
[139] S. Jiang, T. Hu, J. Gild, N. Zhou, J. Nie, M. Qin, T. Harrington, K. Vecchio, J. Luo,
Scr. Mater. 142 (2018) 116–120.
[140] Y. Sharma, B.L. Musico, X. Gao, C. Hua, A.F. May, A. Herklotz, A. Rastogi,
D. Mandrus, J. Yan, H.N. Lee, M.F. Chisholm, V. Keppens, T.Z. Ward, Phys. Rev. B
Condens. Matter Mater. Phys. 2 (2018), 060404.
[141] D.A. Vinnik, E.A. Trofimov, V.E. Zhivulin, S.A. Gudkova, O.V. Zaitseva, D.
A. Zherebtsov, A.Y. Starikov, D.P. Sherstyuk, A.A. Amirov, A.V. Kalgin, S.
V. Trukhanov, F.V. Podgornov, Nanomaterials 10 (2020) 268.
[142] M. Biesuz, S. Fu, J. Dong, A. Jiang, D. Ke, Q. Xu, D. Zhu, M. Bortolotti, M.J. Reece,
C. Hu, S. Grasso, J. Asian Ceram. Soc. 7 (2019) 127–132.
[143] L. Li, Z. Xiang, M. Gao, C. Bian, M. Su, F. Li, X. Xing, Y. Song, iScience 17 (2019)
1–9.
[144] K. Wang, B. Ma, T. Li, C. Xie, Z. Sun, D. Liu, J. Liu, L. An, Ceram. Int. 46 (2020)
18358–18361.
[145] J. Liu, K. Ren, C. Ma, H. Du, Y. Wang, Ceram. Int. 46 (2020) 20576–20581.
[146] R.K. Patel, S.K. Ojha, S. Kumar, A. Saha, P. Mandal, J.W. Freeland, S. Middey,
Appl. Phys. Lett. 116 (2020), 071601.
[147] Z. Zhao, H. Chen, H. Xiang, F.Z. Dai, X. Wang, W. Xu, K. Sun, Z. Peng, Y. Zhou,
J. Mater. Sci. Technol. 47 (2020) 45–51.
[148] R. Zachariasz, D. Bochenek, Eur. Phys. J. B 88 (2015) 296.
[149] Y. Pu, Q. Zhang, R. Li, M. Chen, X. Du, S. Zhou, Appl. Phys. Lett. 115 (2019),
223901.
[150] D. Bochenek, P. Niemiec, R. Skulski, M. Adamczyk-Habrajska, J. Phys. Chem.
Solids 133 (2019) 128–134.
[151] S. Zhou, Y. Pu, Q. Zhang, R. Shi, X. Guo, W. Wang, J. Ji, T. Wei, T. Ouyang,
Ceram. Int. 46 (2020) 7430–7437.
[152] Y. Sharma, Q. Zheng, A.R. Mazza, E. Skoropata, T. Heitmann, Z. Gai, B. Musico, P.
F. Miceli, B.C. Sales, V. Keppens, M. Brahlek, T.Z. Ward, Phys. Rev. Mater. 4
(2020), 014404.
[153] J. Yan, D. Wang, X. Zhang, J. Li, Q. Du, X. Liu, J. Zhang, X. Qi, J. Mater. Sci. 55
(2020) 6942–6951.
[154] V.M. Goldschmidt, Naturwissenschaften 14 (1926) 477–485.
[155] N. Ramadass, Mater. Sci. Eng. 36 (1978) 231–239.
[156] H. Chen, N. Qiu, B. Wu, Z. Yang, S. Sun, Y. Wang, RCS Adv. 10 (2020)
9736–9744.
[157] M. Stygar, J. Dąbrowa, M. Moździerz, M. Zajusz, W. Skubida, K. Mroczka,
K. Berent, K. Świerczek, M. Danielewski, J. Eur. Ceram. Soc. 40 (2020)
1644–1650.
[158] Z. Grzesik, G. Smoła, M. Miszczak, M. Stygar, J. Dąbrowa, M. Zajusz,
K. Świerczek, M. Danielewski, J. Eur. Ceram. Soc. 40 (2020) 835–839.
[159] A. Mao, F. Quan, H.Z. Xiang, Z.G. Zhang, K. Kuramoto, A.L. Xia, J. Mol. Struct.
1194 (2019) 11–18.
[160] A. Mao, H.X. Xie, H.Z. Xiang, Z.G. Zhang, H. Zhang, S. Ran, J. Magn. Magn. Mater.
503 (2020), 166594.
[161] A. Mao, H.Z. Xiang, Z.G. Zhang, K. Kuramoto, H. Zhang, Y. Jia, J. Magn. Magn.
Mater. 497 (2020), 165884.
[162] M.S. Lal, R. Sundara, ACS Appl. Mater. Interfaces 11 (2019) 30846–30857.
[163] T. Parida, A. Karati, K. Guruvidyathri, B.S. Murty, G. Markandeyulu, Scr. Mater.
178 (2020) 513–517.
[164] J. Dąbrowa, M. Stygar, A. Mikuła, A. Knapik, K. Mroczka, W. Tejchman,
M. Danielewski, M. Martin, Mater. Lett. 216 (2018) 32–36.
[165] M. Zamani, E. Naderi, M. Aghajanzadeh, M. Naseri, A. Sharafi, H. Danafar, J. Mol.
Liq. 274 (2019) 60–67.
[166] S. Karimi, P. Kameli, H. Ahmadvand, H. Salamati, Ceram. Int. 42 (2016)
16948–16955.
[167] S.S. Deshmukh, A.V. Humbe, A. Kumar, R.G. Dorik, K.M. Jadhav, J. Alloys.
Compd. 704 (2017) 227–236.
[168] K. Tomiyasu, J. Fukunaga, H. Suzuki, Phys. Rev. B 70 (2004), 214434.
[169] Z. Tian, C. Zhu, J. Wang, Z. Xia, Y. Liu, S. Yuan, J. Magn. Magn. Mater. 377
(2015) 176–182.
[170] A. Manikandan, L.J. Kennedy, M. Bououdina, J.J. Vijaya, J. Magn. Magn. Mater.
349 (2014) 249–258.
[171] A. Ghasemi, S. Ekhlasi, M. Mousavinia, J. Magn. Magn. Mater. 354 (2014)
136–145.
[172] D. Akahoshi, S. Koshikawa, T. Nagase, E. Wada, K. Nishina, R. Kajihara,
H. Kuwahara, T. Saito, Phys. Rev. B 96 (2017), 184419.
[173] M. Fracchia, M. Manzoli, U. Anselmi-Tamburini, P. Ghigna, Scr. Mater. 188
(2020) 26–31.
[174] Z. Teng, L. Zhu, Y. Tan, S. Zeng, Y. Xia, Y. Wang, H. Zhang, J. Eur. Ceram. Soc. 40
(2020) 1639–1643.
[175] A.J. Wright, Q. Wang, S.T. Ko, K.M. Chung, R. Chen, J. Luo, Scr. Mater. 181
(2020) 76–81.
[176] Z. Zhao, H. Xiang, F.Z. Dai, Z. Peng, Y. Zhou, J. Mater. Sci. Technol. 35 (2019)
2647–2651.
S. Akrami et al.
[177] K. Ren, Q. Wang, G. Shao, X. Zhao, Y. Wang, Scr. Mater. 178 (2020) 382–386.
[178] J. Wu, X. Wei, N.P. Padture, P.G. Klemens, M. Gell, E. García, P. Miranzo, M.
I. Osendi, J. Am. Ceram. Soc. 85 (2002) 3031–3035.
[179] M. Zhao, W. Pan, C. Wan, Z. Qu, Z. Li, J. Yang, J. Eur. Ceram. Soc. 37 (2017)
1–13.
[180] L. Yang, C. Zhu, Y. Sheng, H. Nian, Q. Li, P. Song, W. Lu, J. Yang, B. Liu, J. Am.
Ceram. Soc. 102 (2019) 2830–2840.
[181] J.M. Pruneda, E. Artacho, Phys. Rev. B 72 (2005), 085107.
[182] B. Liu, J.Y. Wang, F.Z. Li, Y.C. Zhou, Acta Mater. 58 (2010) 4369–4377.
[183] J. Yang, M. Shahid, M. Zhao, J. Feng, C. Wan, W. Pan, J. Alloys. Compd. 663
(2016) 834–841.
[184] R. Vassen, X. Cao, F. Tietz, D. Basu, D. Stöver, J. Am. Ceram. Soc. 83 (2000)
2023–2028.
[185] D.R. Clarke, S.R. Phillpot, Mater. Today 8 (2005) 22–29.
[186] M.R. Winter, D.R. Clarke, J. Am. Ceram. Soc. 90 (2007) 533–540.
[187] W. Pan, S.R. Phillpot, C. Wan, A. Chernatynskiy, Z. Qu, MRS Bull. 37 (2012)
917–922.
[188] W. Pan, C.L. Wan, Q. Xu, J.D. Wang, Z.X. Qu, Thermochim. Acta 455 (2007)
16–20.
[189] C. Wan, Z. Qu, A. Du, W. Pan, Acta Mater. 57 (2009) 4782–4789.
[190] Z.G. Liu, J.H. Ouyang, Y. Zhou, J. Alloys. Compd. 472 (2009) 319–324.
[191] H. Zhang, K. Sun, Q. Xu, F. Wang, L. Liu, J. Rare Earths 27 (2009) 222–226.
[192] C. Wan, W. Zhang, Y. Wang, Z. Qu, A. Du, R. Wu, W. Pan, Acta Mater. 58 (2010)
6166–6172.
[193] C. Wan, Z. Qu, A. Du, W. Pan, J. Am. Ceram. Soc. 94 (2011) 592–596.
[194] Y. Wang, F. Yang, P. Xiao, Appl. Phys. Lett. 102 (2013), 141902.
[195] K.P. Tseng, Q. Yang, S.J. McCormack, W.M. Kriven, J. Am. Ceram. Soc. 103
(2020) 569–576.
[196] A. Kirnbauer, C. Spadt, C.M. Koller, S. Kolozsvári, P.H. Mayrhofer, Vacuum 168
(2019), 108850.
[197] Y. Dong, K. Ren, Y. Lu, Q. Wang, J. Liu, Y. Wang, J. Eur. Ceram. Soc. 39 (2019)
2574–2579.
[198] X. Ren, Z. Tian, J. Zhang, J. Wang, Scr. Mater. 168 (2019) 47–50.
[199] H. Chen, H. Xiang, F.Z. Dai, J. Liu, Y. Zhou, J. Mater. Sci. Technol. 36 (2020)
134–139.
[200] D.A. Vinnik, E.A. Trofimov, V.E. Zhivulin, O.V. Zaitseva, D.A. Zherebtsov, A.
Y. Starikov, D.P. Sherstyuk, S.A. Gudkova, S.V. Taskaev, Ceram. Int. 46 (2020)
9656–9660.
[201] M.I. Lin, M.H. Tsai, W.J. Shen, J.W. Yeh, Thin Solid Films 518 (2010) 2732–2737.
[202] N. Shankhwar, A. Srinivasan, Mater. Sci. Eng. C 62 (2016) 190–196.
[203] A. Cestari, J. Dent. 55 (2016) 105–113.
[204] Z. Lei, X. Liu, R. Li, H. Wang, Y. Wu, Z. Lu, Scr. Mater. 146 (2018) 340–343.
[205] A. Radoń, Ł. Hawełek, D. Łukowiec, J. Kubacki, P. Włodarczyk, Sci. Rep. 9 (2019)
20078.
[206] J. Zhang, X. Zhang, Y. Li, Q. Du, X. Liu, X. Qi, Mater. Lett. 244 (2019) 167–170.
[207] Z. Ding, J. Bian, S. Shuang, X. Liu, Y. Hu, C. Sun, Y. Yang, Adv. Sustain. Syst. 4
(2020), 1900105.
[208] C.H. Tsau, Y.C. Yang, C.C. Lee, L.Y. Wu, H.J. Huang, Procedia Eng. 36 (2012)
246–252.
[209] B. Gwalani, R.M. Pohan, J. Lee, B. Lee, R. Banerjee, H.J. Ryu, S.H. Hong, Sci. Rep.
8 (2018) 14085.
[210] N. Qiu, H. Chen, Z. Yang, S. Sun, Y. Wang, Y. Cui, J. Alloys. Compd. 777 (2019)
767–774.
[211] B. Cheng, H. Lou, A. Sarkar, Z. Zeng, F. Zhang, X. Chen, L. Tan, V. Prakapenka,
E. Greenberg, J. Wen, R. Djenadic, H. Hahn, Q. Zeng, Commun. Chem. 2 (2019)
114.
[212] Y. Yang, W. Wang, G.Y. Gan, X.F. Shi, B.Y. Tang, Physica B Condens. Matter 550
(2018) 163–170.
[213] I. Kunce, M. Polanski, J. Bystrzycki, Int. J. Hydrogen Energy 38 (2013)
12180–12189.
[214] D. Karlsson, G. Ek, J. Cedervall, C. Zlotea, K.T. Møller, T.C. Hansen, J. Bednarcik,
M. Paskevicius, M.H. Sørby, T.R. Jensen, U. Jansson, M. Sahlberg, Inorg. Chem.
57 (2018) 2103–2110.
[215] G. Zepon, D.R. Leiva, R.B. Strozi, A. Bedoch, S.J.A. Figueroa, T.T. Ishikawa, W.
J. Botta, Int. J. Hydrogen Energy 43 (2018) 1702–1708.
[216] E.M. Dematteis, A. Santoru, M.G. Poletti, C. Pistidda, T. Klassen, M. Dornheim,
M. Baricco, Int. J. Hydrogen Energy 43 (2018) 16793–16803.
[217] H. Shen, J. Hu, P. Li, G. Huang, J. Zhang, J. Zhang, Y. Mao, H. Xiao, X. Zhou,
X. Zu, X. Long, S. Peng, J. Mater. Sci. Technol. 55 (2020) 116–125.
[218] I. Kunce, M. Polanski, J. Bystrzycki, Int. J. Hydrogen Energy 39 (2014)
9904–9910.
[219] M. Sahlberg, D. Karlsson, C. Zlotea, U. Jansson, Sci. Rep. 6 (2016) 36770.
[220] S. Yang, F. Yang, C. Wu, Y. Chen, Y. Mao, L. Luo, J. Alloys. Compd. 663 (2016)
460–465.
[221] I. Kunce, M. Polański, T. Czujko, Int. J. Hydrogen Energy 42 (2017)
27154–27164.
[222] C. Zlotea, M.A. Sow, G. Ek, J.P. Couzinié, L. Perrière, I. Guillot, J. Bourgon, K.
T. Møller, T.R. Jensen, E. Akiba, M. Sahlberg, J. Alloys. Compd. 775 (2019)
667–674.
[223] M.M. Nygård, G. Ek, D. Karlsson, M.H. Sørby, M. Sahlberg, B.C. Hauback, Acta
Mater. 175 (2019) 121–129.
[224] M.M. Nygård, G. Ek, D. Karlsson, M. Sahlberg, M.H. Sørby, B.C. Hauback, Int. J.
Hydrogen Energy 44 (2019) 29140–29149.
[225] J. Hu, H. Shen, M. Jiang, H. Gong, H. Xiao, Z. Liu, G. Sun, X. Zu, Nanomaterials 9
(2019) 461.
57
Materials Science & Engineering R 146 (2021) 100644
[226] J. Montero, G. Ek, L. Laversenne, V. Nassif, G. Zepon, M. Sahlberg, C. Zlotea,
J. Alloys. Compd. 835 (2020), 155376.
[227] S.K. Dewangan, V.K. Sharma, P. Sahu, V. Kumar, Int. J. Hydrogen Energy 45
(2020) 16984–16991.
[228] F.Z. Dai, B. Wen, Y. Sun, H. Xiang, Y. Zhou, J. Mater. Sci. Technol. 43 (2020)
168–174.
[229] C.M. Handley, J. Behler, Eur. Phys. J. B 87 (2014) 152.
[230] J. Behler, Int. J. Quantum Chem. 115 (2015) 1032–1050.
[231] A.P. Bartók, G. Csányi, Int. J. Quantum Chem. 115 (2015) 1051–1057.
[232] J. Behler, J. Chem. Phys. 145 (2016), 170901.
[233] H. Huang, L. Shao, H. Liu, Phys. Status Solidi B 258 (2021), 2100140.
[234] D.G. Sangiovanni, F. Tasnádi, T. Harrington, M. Odén, K.S. Vecchio, I.
A. Abrikosov, Mater. Des. 204 (2021), 109634.
[235] J. Zhang, J. Hu, H. Xiao, H. Shen, L. Xie, G. Sun, X. Zu, Metals 11 (2021) 553.
[236] J. Hu, J. Zhang, H. Xiao, L. Xie, G. Sun, H. Shen, P. Li, J. Zhang, X. Zu, Int. J.
Hydrogen Energy 4 (6) (2021) 21050–21058.
[237] J. Hu, J. Zhang, H. Xiao, L. Xie, G. Sun, H. Shen, P. Li, J. Zhang, X. Zu, J. Alloys.
Compd. 879 (2021), 160482.
[238] A.L. Vyatskikh, B.E. MacDonald, A.D. Dupuy, E.J. Lavernia, J.M. Schoenung,
H. Hahn, Scr. Mater. 201 (2021), 113914.
[239] X.T. Chen, L. Shao, T.W. Fan, N. Ding, J. Yang, B.Y. Tang, J. Solid State Chem. 303
(2021), 122469.
[240] Z. Rák, J.P. Maria, D.W. Brenner, Mater. Lett. 217 (2018) 300–303.
[241] L. Kong, X. Chen, B.Q. Li, H.J. Peng, J.Q. Huang, J. Xie, Q. Zhang, Adv. Mater. 30
(2018), 1705219.
[242] J.D. Grice, R.B. Ferguson, Canad. Mineral. 12 (1974) 248–252.
[243] L.K. Bhaskar, V. Nallathambi, R. Kumar, J. Am. Ceram. Soc. 103 (2020)
3416–3424.
[244] G. Wu, S. Seebold, E. Zayhenskikh, K. Hack, M. Müller, A structure-based
viscosity model and database for multicomponent oxide melts, in: R.G. Reddy,
P. Chaubal, P.C. Pistorius, U. Pal (Eds.), Advances in Molten Slags, Fluxes, and
Salts: Proceedings of the 10th International Conference on Molten Slags, Fluxes
and Salts, Springer, 2016, pp. 397–404.
[245] K. Hack, G. Wu, E. Yazhenskikh, T. Jantzen, M. Müller, Calphad 65 (2019)
101–110.
[246] A.S. Vusikhis, D.Z. Kudinov, L.I. Leont’ev, Russ. J. Phys. Chem. A 82 (2008)
1824–1827.
[247] M. Edén, J. Non-Cryst. Solids 357 (2011) 1595–1602.
[248] V.S. Rudnev, S. Wybornov, I.V. Lukiyanchuk, I.V. Chernykh, Prot. Met. Phys.
Chem. Surf. 50 (2014) 191–194.
[249] A.S. Vusikhis, L.I. Leont’ev, V.P. Chentsov, D.Z. Kudinov, E.N. Selivanov, Steel
Transl. 47 (2017) 21–25.
[250] A.S. Vusikhis, L.I. Leont’ev, V.P. Chentsov, D.Z. Kudinov, E.N. Selivanov, Steel
Transl. 47 (2017) 772–776.
[251] S. Hechler, B. Ruta, M. Stolpe, E. Pineda, Z. Evenson, O. Gross, A. Bernasconi,
R. Busch, I. Gallino, Phys. Rev. Mater 2 (2018), 085603.
[252] C. Liu, H. Ni, S. Yang, J. Li, F. Ye, Ironmak. Steelmak. 45 (2018) 195–203.
[253] B.R. Gelchinskii, E.V. Dyul’dina, V.N. Selivanov, L.I. Leontiev, Dokl. Phys. Chem.
485 (2019) 43–46.
[254] B.R. Gel’chinskii, E.V. Dyul’dina, L.I. Leont’ev, Steel Transl. 49 (2019) 601–605.
[255] E.V. Dyul’dina, B.R. Gel’chinskii, V.N. Selivanov, Russ. Metall. 2019 (2019)
119–121.
[256] G. Anand, A.P. Wynn, C.M. Handley, C.L. Freeman, Acta Mater. 146 (2018)
119–125.
[257] D.R. Cassar, A.C.P.L.F. de Carvalho, E.D. Zanotto, Acta Mater. 159 (2018)
249–256.
[258] B. Ye, T. Wen, M.C. Nguyen, L. Hao, C.Z. Wang, Y. Chu, Acta Mater. 170 (2019)
15–23.
[259] Q. Zhang, J. Zhang, N. Li, W. Chen, J. Appl. Phys. 126 (2019), 025101.
[260] H. Zhang, D. Hedman, P. Feng, G. Han, F. Akhtar, Dalton Trans. 48 (2019)
5161–5167.
[261] S. Jiang, L. Shao, T. Fan, J.M. Duan, X.T. Chen, B.Y. Tang, Int. J. Quantum Chem.
121 (2020), e26509.
[262] S. Zhao, J. Am. Ceram. Soc. 104 (2020) 1874–1886.
[263] L. Backman, J. Gild, J. Luo, E.J. Opila, Acta Mater. 197 (2020) 20–27.
[264] L. Backman, J. Gild, J. Luo, E.J. Opila, Acta Mater. 197 (2020) 81–90.
[265] X.F. Wei, Y. Qin, J.X. Liu, F. Li, Y.C. Liang, G.J. Zhang, J. Eur. Ceram. Soc. 40
(2020) 935–941.
[266] K. Kaufmann, D. Maryanovsky, W.M. Mellor, C. Zhu, A.S. Rosengarten, T.
J. Harrington, C. Oses, C. Toher, S. Curtarolo, K.S. Vecchio, Npj Comput. Mater. 6
(2020) 42.
[267] P. Sarker, T. Harrington, C. Toher, C. Oses, M. Samiee, J.P. Maria, D.W. Brenner,
K.S. Vecchio, S. Curtarolo, Nat. Commun. 9 (2018) 4980.
[268] A. Kirnbauer, A. Kretschmer, C.M. Koller, T. Wojcik, V. Paneta, M. Hans, J.
M. Schneider, P. Polcik, P.H. Mayrhofer, Surf. Coat. Technol. 389 (2020), 125674.
[269] Y.P. Wang, G.Y. Gan, W. Wang, Y. Yang, B.Y. Tang, Phys. Status Solidi B 255
(2018), 1800011.
[270] F.Z. Dai, Y. Sun, B. Wen, H. Xiang, Y. Zhou, J. Mater. Sci. Technol. 72 (2021)
8–15.
[271] P. Edalati, R. Floriano, A. Mohammadi, Y. Li, G. Zepon, H.W. Li, K. Edalati, Scr.
Mater. 178 (2020) 387–390.
[272] R. Ramprasad, R. Batra, G. Pilania, A. Mannodi-Kanakkithodi, C. Kim, Npj
Comput. Mater. 3 (2017) 54.
[273] L.M. Ghiringhelli, J. Vybiral, S.V. Levchenko, C. Draxl, M. Scheffler, Phys. Rev.
Lett. 114 (2015), 105503.
S. Akrami et al. Materials Science & Engineering R 146 (2021) 100644

[274] L. Spiridigliozzi, C. Ferone, R. Cioffi, G. Dell’Agli, Acta Mater. 202 (2021) [327] Y. Zhang, J. Nie, J. Luo, J. Ceram. Soc. Japan 124 (2016) 296–300.
181–189. [328] Y. Zhang, J. Nie, J.M. Chan, J. Luo, Acta Mater. 125 (2017) 465–475.
[275] T.J. Harrington, J. Gild, P. Sarker, C. Toher, C.M. Rost, O.F. Dippo, C. McElfresh, [329] M. Biesuz, V.M. Sglavo, J. Eur. Ceram. Soc. 39 (2019) 115–143.
K. Kaufmann, E. Marin, L. Borowski, P.E. Hopkins, J. Luo, S. Curtarolo, D. [330] M. Yu, S. Grasso, R. Mckinnon, T. Saunders, M.J. Reece, Adv. Appl. Ceram. 116
W. brenner, K.S. Vecchio, Acta Mater. 166 (2019) 271–280. (2017) 24–60.
[276] S. Ning, T. Wen, B. Ye, Y. Chu, J. Am. Ceram. Soc. 103 (2020) 2244–2251. [331] Y. Zhang, S.K. Sun, W. Zhang, Y. You, W.M. Guo, Z.W. Chen, J.H. Yuan, H.T. Lin,
[277] D. Liu, H. Liu, S. Ning, Y. Chu, J. Adv. Ceram. 9 (2020) 339–348. Ceram. Int. 46 (2020) 14299–14303.
[278] R. Floriano, G. Zepon, K. Edalati, G.L.B.G. Fontana, A. Mohammadi, Z. Ma, H. [332] D. Liu, T. Wen, B. Ye, Y. Chu, Scr. Mater. 167 (2019) 110–114.
W. Li, R.J. Contieri, Int. J. Hydrogen Energy 45 (2020) 33759–33770. [333] J. Gild, A. Wright, K. Quiambao-Tomko, M. Qin, J.A. Tomko, M.S. bin Hoque, J.
[279] Y. Xia, P. Yang, Y. Sun, Y. Wu, B. Mayers, B. Gates, Y. Yin, F. Kim, H. Yan, Adv. L. Braun, B. Bloomfield, D. Martinez, T. Harrington, K. Vecchio, P.E. Hopkins,
Mater. 15 (2003) 353–389. J. Luo, Ceram. Int. 46 (2020) 6906–6913.
[280] Y. Chu, S. Jing, X. Yu, Y. Zhao, Cryst. Growth Des. 18 (2018) 2941–2947. [334] Y. Zhang, Z.B. Jiang, S.K. Sun, W.M. Guo, Q.S. Chen, J.X. Qiu, K. Plucknett, H.
[281] E. Chicardi, C. García-Garrido, J. Hernández-Saz, F.J. Gotor, Ceram. Int. 46 T. Lin, J. Eur. Ceram. Soc. 39 (2019) 3920–3924.
(2020) 21421–21430. [335] L. Feng, W.G. Fahrenholtz, G.E. Hilmas, J. Eur. Ceram. Soc. 40 (2020)
[282] Q. Zhao, J. Mei, W. Jin, Q. Jiang, J. Am. Ceram. Soc. 103 (2020) 4733–4737. 3815–3823.
[283] D.O. Moskovskikh, S. Vorotilo, A.S. Sedegov, K.V. Kuskov, K.V. Bardasova, P. [336] D. Liu, H. Liu, S. Ning, B. Ye, Y. Chu, J. Am. Ceram. Soc. 102 (2019) 7071–7076.
V. Kiryukhantsev-korneev, M. Zhukovskyi, A.S. Mukasyan, Ceram. Int. 46 (2020) [337] L. Feng, W.G. Fahrenholtz, G.E. Hilmas, J. Am. Ceram. Soc. 103 (2020) 724–730.
19008–19014. [338] J. Gu, J. Zou, S.K. Sun, H. Wang, S.Y. Yu, J. Zhang, W. Wang, Z. Fu, Sci. China
[284] R.Z. Valiev, Y. Estrin, Z. Horita, T.G. Langdon, M.J. Zechetbauer, Y.T. Zhu, JOM Mater. 62 (2019) 1898–1909.
58 (4) (2006) 33–39. [339] F. Li, Y. Lu, X.G. Wang, W. Bao, J.X. Liu, F. Xu, G.J. Zhang, Ceram. Int. 45 (2019)
[285] A.P. Zhilyaev, T.G. Langdon, Prog. Mater. Sci. 53 (2008) 893–979. 22437–22441.
[286] K. Edalati, Z. Horita, Mater. Sci. Eng. A 652 (2016) 325–352. [340] L. Feng, W.G. Fahrenholtz, G.E. Hilmas, J. Am. Ceram. Soc. 102 (2019)
[287] J.K. Han, J.I. Jang, T.G. Langdon, M. Kawasaki, Mater. Trans. 60 (2019) 7217–7224.
1131–1138. [341] H. Chen, H. Xiang, F.Z. Dai, J. Liu, Y. Zhou, J. Mater. Sci. Technol. 35 (2019)
[288] K. Edalati, Mater. Trans. 60 (2019) 1221–1229. 2404–2408.
[289] A. Bachmaier, R. Pippan, Mater. Trans. 60 (2019) 1256–1269. [342] I.P. Borovinskaya, A.A. Gromov, E.A. Levashov, Y.M. Maksimov, A.S. Mukasyan,
[290] K. Edalati, Y. Yokoyama, Z. Horita, Mater. Trans. 51 (2010) 23–26. A.S. Rogachev (Eds.), Concise Encyclopedia of Self-Propagating High-
[291] H. Asgharzadeh, S.H. Joo, H.S. Kim, Metall. Mater. Trans. A 45 (2014) Temperature Synthesis: History, Theory, Technology, and Products, first ed.,
4129–4137. Elsevier Inc., 2017.
[292] K. Edalati, H. Emami, Y. Ikeda, H. Iwaoka, I. Tanaka, E. Akiba, Z. Horita, Acta [343] A.S. Mukasyan, B.B. Khina, R.V. Reeves, S.F. Son, Chem. Eng. J. 174 (2011)
Mater. 108 (2016) 293–303. 677–686.
[293] A. Mazilkin, B. Straumal, A. Kilmametov, P. Straumal, B. Baretzky, Mater. Trans. [344] C.E. Shuck, K.V. Manukyan, S. Rouvimov, A.S. Rogachev, A.S. Mukasyan,
60 (2019) 1489–1499. Combust. Flame 163 (2016) 487–493.
[294] H. Razavi-Khosroshahi, K. Edalati, M. Hirayama, H. Emami, M. Arita, [345] P.R. Bonneau, J.B. Wiley, R.B. Kaner, M.F. Mansuktto, Inorg. Syn. 30 (1995)
M. Yamauchi, H. Hagiwara, S. Ida, T. Ishihara, E. Akiba, Z. Horita, M. Fuji, ACS 33–37.
Catal. 6 (2016) 5103–5107. [346] M. Pini, R. Rosa, P. Neri, F. Bondioli, A.M. Ferrari, Green Chem. 17 (2015)
[295] K. Edalati, Adv. Eng. Mater. 21 (2019), 1800272. 518–531.
[296] K. Edalati, H.W. Li, A. Kilmametov, R. Floriano, C. Borchers, Metals 11 (2021) [347] G. Tallarita, R. Licheri, S. Garroni, R. Orrù, G. Cao, Scr. Mater. 158 (2019)
1263. 100–104.
[297] P. Edalati, Q. Wang, H. Razavi-Khosroshahi, M. Fuji, T. Ishihara, K. Edalati, [348] A. Cestari, L.R. Avila, E.C.O. Nassor, P.F. dos Santos Pereira, P.S. Calefi, K.
J. Mater. Chem. A Mater. Energy Sustain. 8 (2020) 3814–3821. J. Ciuffi, S. Nakagaki, A.C.P. Gomes, E.J. Nassar, Mater. Res. 12 (2009) 139–143.
[298] P. Edalati, X.F. Shen, M. Watanabe, T. Ishihara, M. Arita, M. Fuji, K. Edalati, [349] Z. Zhang, S. Yang, X. Hu, H. Xu, H. Peng, M. Liu, B.P. Thapaliya, K. Jie, J. Zhao,
J. Mater. Chem. A 9 (2021) 15076–15086. J. Liu, H. Chen, Y. Leng, X. Lu, J. Fu, P. Zhang, S. Dai, Chem. Mater. 31 (2019)
[299] M.O. de Marco, Y. Li, H.W. Li, K. Edalati, R. Floriano, Adv. Eng. Mater. 22 (2020), 5529–5536.
1901079. [350] F.T. Li, J. Ran, M. Jaroniec, S.Z. Qiao, Nanoscale 7 (2015) 17590–17610.
[300] M. Qin, J. Gild, H. Wang, T. Harrington, K.S. Vecchio, J. Luo, J. Eur. Ceram. Soc. [351] N.R. de Tacconi, H.K. Timmaji, W. Chanmanee, M.N. Huda, P. Sarker, C. Janáky,
40 (2020) 4348–4353. K. Rajeshwar, ChemPhysChem 13 (2012) 2945–2955.
[301] R.F. Guo, H.R. Mao, Z.T. Zhao, P. Shen, Scr. Mater. 193 (2021) 103–107. [352] M. Lackner (Ed.), Combustion Synthesis: Novel Routes to Novel Materials, first
[302] D. Lin, K.W. Kwok, Curr. Appl. Phys. 9 (2009) 1369–1374. ed., Bentham Science Publishers, 2010.
[303] B. Ye, T. Wen, D. Liu, Y. Chu, Corros. Sci. 153 (2019) 327–332. [353] F.T. Li, Y. Liu, Z.M. Sun, Y. Zhao, R.H. Liu, L.J. Chen, D.S. Zhao, Catal. Sci.
[304] B. Ye, T. Wen, Y. Chu, J. Am. Ceram. Soc. 103 (2020) 500–507. Technol. 2 (2012) 1455–1462.
[305] S. Grasso, T. Saunders, H. Porwal, B. Milsom, A. Tudball, M. Reece, J. Am. Ceram. [354] A.V. Saghir, S.M. Beidokhti, J.V. Khaki, A. Salimi, J. Eur. Ceram. Soc. 41 (2021)
Soc. 99 (2016) 1534–1543. 563–579.
[306] S. Grasso, E.Y. Kim, T. Saunders, M. Yu, A. Tudball, S.H. Choi, M. Reece, Crys. [355] J. Sushil, A. Kumar, A. Gautam, M.I. Ahmad, Mater. Chem. Phys. 259 (2021),
Growth Des. 16 (2016) 2317–2321. 124014.
[307] B. Niu, F. Zhang, J. Zhang, W. Ji, W. Wang, Z. Fu, Scr. Mater. 116 (2016) [356] Y.W. Chen, J.J. Ruan, J.M. Ting, Y.H. Su, K.S. Chang, Ceram. Int. 47 (2021)
127–130. 11451–11458.
[308] R. McKinnon, S. Grasso, A. Tudball, M.J. Reece, J. Eur. Ceram. Soc. 37 (2017) [357] J. Li, Q. Wu, J. Wu, in: M. Aliofkhazraei (Ed.), Handbook of Nanoparticles, first
2787–2794. ed., Springer International Publishing, Switzerland, 2015.
[309] J. Gild, K. Kaufmann, K. Vecchio, J. Luo, Scr. Mater. 170 (2019) 106–110. [358] G.B. Nair, V.B. Pawade, S.J. Dhoble, in: B.A. Bhanvase, V.B. Pawade, S.J. Dhoble,
[310] G. Franceschin, N. Flores-Martínez, G. Vázquez-Victorio, S. Ammar, S.H. Sonawane, M. Ashokkumar (Eds.), Nanomaterials for Green Energy, Elsevier
R. Valenzuela, in: I. Shishkovsky (Ed.), Sintering of Functional Materials, Inc., 2018, pp. 411–431.
IntechOpen, 2018. [359] D.J. Fray, Int. Mater. Rev. 53 (2008) 317–325.
[311] X.Q. Shen, J.X. Liu, F. Li, G.J. Zhang, Ceram. Int. 45 (2019) 24508–24514. [360] D. Wang, X. Jin, G.Z. Chen, Annu. Rep. Prog. Chem. 104 (2008) 189–234.
[312] X.G. Wang, J.X. Liu, Y.M. Kan, G.J. Zhang, J. Eur. Ceram. Soc. 32 (2012) [361] K. Mohandas, Min. Proc. Ext. Met. 122 (2013) 195–212.
1795–1802. [362] D. Fray, C. Schwandt, Mater. Trans. 58 (2017) 306–312.
[313] X. Yan, L. Constantin, Y. Lu, J.F. Silvain, M. Nastasi, B. Cui, J. Am. Ceram. Soc. [363] X.Y. Yan, M.I. Pownceby, M.A. Cooksey, M.R. Lanyon, Min. Proc. Ext. Met. 118
101 (2018) 4486–4491. (2009) 23–34.
[314] X.F. Wei, J.X. Liu, F. Li, Y. Qin, Y.C. Liang, G.J. Zhang, J. Eur. Ceram. Soc. 39 [364] A.M. Abdelkader, D.J. Fray, J. Eur. Ceram. Soc. 32 (2012) 4481–4487.
(2019) 2989–2994. [365] Q. Song, Q. Xu, J. Meng, T. Lou, Z. Ning, Y. Qi, K. Yu, J. Alloys. Compd. 647
[315] A. Bellosi, F. Monteverde, D. Sciti, Int. J. Appl. Ceram. Technol. 3 (2006) 32–40. (2015) 245–251.
[316] S. Grasso, Y. Sakka, J. Ceram. Soc. Japan 121 (2013) 524–526. [366] G. Sun, H. Yang, C. Ma, Y. Zhang, J. Yu, W. He, X. Song, New J. Chem. 39 (2015)
[317] O. Vasylkiv, H. Borodianska, Y. Sakka, J. Eur. Ceram. Soc. 28 (2008) 919–927. 7012–7018.
[318] D. Demirskyi, O. Vasylkiv, Ceram. Int. 42 (2016) 16396–16400. [367] J. Fan, Y. Yang, D. Tang, W. Xiao, X. Mao, D. Wang, J. Electrochem. Soc. 164
[319] V. Mamedov, Powder Metall. 45 (2002) 322–328. (2017) E144.
[320] S.K. Sun, G.J. Zhang, W.W. Wu, J.X. Liu, T. Suzuki, Y. Sakka, Scr. Mater. 69 [368] J. Sure, D. Sri Maha Vishnu, H.K. Kim, C. Schwandt, Angew. Chem. 132 (2020)
(2013) 139–142. 11928–11933.
[321] O. Vasylkiv, H. Borodianska, P. Badica, S. Grasso, Y. Sakka, A. Tok, L.T. Su, [369] M.A. Gülgün, M.H. Nguyen, W.M. Kriven, J. Am. Ceram. Soc. 82 (1999) 556–560.
M. Bosman, J. Ma, J. Nanosci. Nanotechnol. 12 (2012) 959–965. [370] M.H. Nguyen, S.J. Lee, W.M. Kriven, J. Mater. Res. 14 (1999) 3417–3426.
[322] H. Wang, Y. Cao, W. Liu, Y. Wang, Ceram. Int. 46 (2020) 11160–11168. [371] F. Qu, Y. Yuan, M. Yang, Chem. Mater. 29 (2017) 969–974.
[323] Y. Tan, C. Chen, S. Li, X. Han, J. Xue, T. Liu, X. Zhou, H. Zhang, J. Alloys. Compd. [372] T. Jin, X. Sang, R.R. Unocic, R.T. Kinch, X. Liu, J. Hu, H. Liu, S. Dai, Adv. Mater.
816 (2020), 152523. 30 (2018), 1707512.
[324] G. Tallarita, R. Licheri, S. Garroni, S. Barbarossa, R. Orru, G. Cao, J. Eur. Ceram. [373] D.H.A. Blank, M. Dekkers, G. Rijnders, J. Phy. D: Appl. Phys. 47 (2013), 034006.
Soc. 40 (2020) 942–952. [374] G. Fang, J. Gao, J. Lv, H. Jia, H. Li, W. Liu, G. Xie, Z. Chen, Y. Huang, Q. Yuan,
[325] M. Cologna, J.S.C. Francis, R. Raj, J. Eur. Ceram. Soc. 31 (2011) 2827–2837. X. Liu, X. Lin, S. Sun, H.J. Qiu, Appl. Catal. B: Environm. 268 (2020), 118431.
[326] X. Hao, Y. Liu, Z. Wang, J. Qiao, K. Sun, J. Power Sources 210 (2012) 86–91.

58
S. Akrami et al.
[375] Y. Sun, F. Chen, W. Qiu, L. Ye, W. Han, W. Zhao, H. Zhou, T. Zhao, J. Am. Ceram.
Soc. 103 (2020) 6081–6087.
[376] R. Djenadic, M. Botros, C. Benel, O. Clemens, S. Indris, A. Choudhary,
T. Bergfeldt, H. Hahn, Solid State Ion. 263 (2014) 49–56.
[377] B. Thiebaut, Platin. Met. Rev. 55 (2011) 149–151.
[378] R. Strobel, A. Baiker, S.E. Pratsinis, Adv. Powder Technol. 17 (2006) 457–480.
[379] R. Strobel, S.E. Pratsinis, Platin. Met. Rev. 53 (2009) 11–20.
[380] M.B. Kumar, S.S. Bhattacharya, Process. Appl. Ceram. 6 (2012) 165–171.
[381] X. Wang, Z. Huang, Y. Yao, H. Qiao, G. Zhong, Y. Pei, C. Zheng, D. Kline, Q. Xia,
Z. Lin, J. Dai, M.R. Zachariah, B. Yang, R. Shahbazian-Yassar, L. Hu, Mater. Today
35 (2020) 106–114.
[382] Y. Zhang, X.H. Yan, W.B. Liao, K. Zhao, Entropy 20 (2018) 624.
[383] K. von Fieandt, L. Riekehr, B. Osinger, S. Fritze, E. Lewin, Surf. Coat. Technol. 389
(2020), 125614.
[384] R. Chen, Z. Cai, J. Pu, Z. Lu, S. Chen, S. Zheng, C. Zeng, J. Alloys. Compd. 827
(2020), 153836.
[385] R. Li, M. Li, C. Jiang, B. Qiao, W. Zhang, J. Xu, J. Alloys. Compd. 773 (2019)
482–489.
[386] T.X. Nguyen, Y.H. Su, J. Hattrick-Simpers, H. Joress, T. Nagata, K.S. Chang,
S. Sarker, A. Mehta, J.M. Ting, ACS Comb. Sci. 22 (2020) 858–866.
[387] P.H. Mayrhofer, A. Kirnbauer, P. Ertelthaler, C.M. Koller, Scr. Mater. 149 (2018)
93–97.
[388] A. Vladescu, I. Titorencu, Y. Dekhtyar, V. Jinga, V. Pruna, M. Balaceanu, M. Dinu,
I. Pana, V. Vendina, M. Braic, PLoS One 11 (2016), e0161151.
[389] P.B. Meisenheimer, T.J. Kratofil, J.T. Heron, Sci. Rep. 7 (2017) 13344.
[390] D. Ma, H. Tan, Y. Zhang, Y. Li, Mater. Trans. 44 (2003) 2007–2010.
[391] Y. Zhang, Z.P. Lu, S.G. Ma, P.K. Liaw, Z. Tang, Y.Q. Cheng, M.C. Gao, MRS
Commun. 4 (2014) 57–62.
[392] S.G. Ma, P.K. Liaw, M.C. Gao, J.W. Qiao, Z.H. Wang, Y. Zhang, J. Alloys. Compd.
604 (2014) 331–339.
[393] H.W. Chang, P.K. Huang, A. Davison, J.W. Yeh, C.H. Tsau, C.C. Yang, Thin Solid
Films 516 (2008) 6402–6408.
[394] Y. Zhang, G. Chen, C. Gan, J. ASTM Int. 7 (5) (2010) 1–8.
[395] Y. Zhang, Mater. Sci. Forum 654-656 (2010) 1058–1061.
[396] Y. Zhang, Y.J. Zhou, Mater. Sci. Forum 561-565 (2007) 1337–1339.
[397] H. Cai, H. Zhang, Y. Zheng, IEEE Trans. Magn. 43 (2007) 2686–2688.
[398] H. Zhang, Y. Pan, Y. He, H. Jiao, Appl. Surf. Sci. 257 (2011) 2259–2263.
[399] C.M. Lin, H.L. Tsai, H.Y. Bor, Intermetallics 18 (2010) 1244–1250.
[400] M.V. Talanov, O.N. Razumovskaya, L.A. Shilkina, L.A. Reznichenko, Inorg. Mater.
Appl. Res. 49 (2013) 957–961.
[401] M. Lim, Z. Rak, J.L. Braun, C.M. Rost, G.N. Kotsonis, P.E. Hopkins, J.P. Maria, D.
W. Brenner, J. Appl. Phys. 125 (2019), 055105.
[402] B. Musicó, Q. Wright, T.Z. Ward, A. Grutter, E. Arenholz, D. Gilbert, D. Mandrus,
V. Keppens, Phys. Rev. Mater. 3 (2019), 104416.
[403] M.V. Talanov, A.A. Pavelko, L.A. Reznichenko, J. Adv. Dielectr. 10 (2020),
2060004.
[404] K. Zhang, W. Li, J. Zeng, T. Deng, B. Luo, H. Zhang, X. Huang, J. Alloys. Compd.
817 (2020), 153328.
[405] A. Pavelko, L. Shilkina, L. Reznichenko, J. Adv. Dielectr. 10 (2020), 2060011.
[406] H. Chen, B. Zhao, Z. Zhao, H. Xiang, F.Z. Dai, J. Liu, Y. Zhou, J. Mater. Sci.
Technol. 47 (2020) 216–222.
[407] M. Pianassola, M. Loveday, J.W. McMurray, M. Koschan, C.L. Melcher,
M. Zhuravleva, J. Am. Ceram. Soc. 103 (2020) 2908–2918.
[408] A. Gautam, M.I. Ahmad, Ceram. Int. 47 (2021) 22225–22228.
[409] A.J. Wright, Q. Wang, C. Hu, Y.T. Yeh, R. Chen, J. Luo, Acta Mater. 211 (2021),
116858.
[410] N.A. Khan, B. Akhavan, Z. Zheng, H. Liu, C. Zhou, H. Zhou, L. Chang, Y. Wang,
Y. Liu, L. Sun, M.M. Bilek, Z. Liu, Appl. Surf. Sci. 553 (2021), 149491.
[411] Y. Liang, B. Luo, H. Dong, D. Wang, Ceram. Int. 47 (2021) 20196–20200.
[412] K. Chen, J. Ma, C. Tan, C. Li, L. An, Ceram. Int. 47 (2021) 21207–21211.
[413] J. Ma, K. Chen, C. Li, X. Zhang, L. An, Ceram. Int. 47 (2021) 24348–24352.
[414] L. Zhou, F. Li, J.X. Liu, S.K. Sun, Y. Liang, G.J. Zhang, J. Hazard. Mater. 415
(2021), 125596.
[415] S. Sun, Z.M. Yang, N. Qiu, H.M. Yang, H. Chen, J.C. Zhang, B. Wu, Y.X. Cao, D.
W. Luo, K. Zhang, Y. Wang, J. Magn. Magn. Mater. 538 (2021), 168271.
[416] Y. Yang, H. Bao, H. Ni, X. Ou, S. Wang, B. Lin, P. Feng, Y. Ling, J. Power Sources
482 (2021), 228959.
[417] X. Zhang, L. Xue, F. Yang, Z. Shao, H. Zhang, Z. Zhao, K. Wang, J. Alloys. Compd.
863 (2021), 158763.
[418] Y. Zhang, W. Dai, P. Zhang, T. Lu, Y. Pan, J. Alloys. Compd. 868 (2021), 159064.
[419] H.R. Mao, R.F. Guo, Y. Cao, S.B. Jin, X.M. Qiu, P. Shen, J. Eur. Ceram. Soc. 41
(2021) 2855–2860.
[420] Z. Teng, Y. Tan, S. Zeng, Y. Meng, C. Chen, X. Han, H. Zhang, J. Eur. Ceram. Soc.
41 (2021) 3614–3620.
[421] E. Bonnet, J.C. Grenier, J.M. Bassat, A. Jacob, B. Delatouche, S. Bourdais, J. Eur.
Ceram. Soc. 41 (2021) 4505–4515.
[422] A.D. Dupuy, M.R. Chellali, H. Hahn, J.M. Schoenung, J. Eur. Ceram. Soc. 41
(2021) 4850–4858.
[423] L. Xu, H. Wang, L. Su, D. Lu, K. Peng, H. Gao, J. Eur. Ceram. Soc. 41 (2021)
6670–6676.
[424] J. He, G. He, J. Liu, J. Tao, J. Eur. Ceram. Soc. 41 (2021) 6080–6086.
[425] J. Cieslak, M. Reissner, K. Berent, J. Dabrowa, M. Stygar, M. Mozdzierz,
M. Zajusz, Acta Mater. 206 (2021), 116600.
[426] M. Mozdzierz, J. Dabrowa, A. Stepien, M. Zajusz, M. Stygar, W. Zaj,
M. Danielewski, K. Swierczek, Acta Mater. 208 (2021), 116735.
59
Materials Science & Engineering R 146 (2021) 100644
[427] C.Y. Huang, C.W. Huang, M.C. Wu, J. Patra, T.X. Nguyen, M.T. Chang,
O. Clemens, J.M. Ting, J. Li, J.K. Chang, W.W. Wu, Chem. Eng. J. 420 (2021),
129838.
[428] Z. Jin, J. Lyu, Y.L. Zhao, H. Li, Z. Chen, X. Lin, G. Xie, X. Liu, J.J. Kai, H.J. Qiu,
Chem. Mater. 33 (2021) 1771–1780.
[429] Y. Sharma, A.R. Mazza, B.L. Musico, E. Skoropata, R. Nepal, R. Jin, A.V. Ievlev,
L. Collins, Z. Gai, A. Chen, M. Brahlek, V. Keppens, T.Z. Ward, ACS Appl. Mater.
Interfaces 13 (2021) 17971–17977.
[430] T.X. Nguyen, Y.C. Liao, C.C. Lin, Y.H. Su, J.M. Ting, Adv. Funct. Mater. 31 (2021),
2101632.
[431] M. Ahn, Y. Park, S.H. Lee, S. Chae, J. Lee, J.T. Heron, E. Kioupakis, W.D. Lu, J.
D. Phillips, Adv. Electron. Mater. 7 (2021), 2001258.
[432] K. Gu, D. Wang, C. Xie, T. Wang, G. Huang, Y. Liu, Y. Zou, L. Tao, S. Wang,
Angew. Chem. (2021) in press.
[433] H. Li, Y. Zhou, Z. Liang, H. Ning, X. Fu, Z. Xu, T. Qiu, W. Xu, R. Yao, J. Peng,
Coatings 11 (2021) 628.
[434] L. Tang, Z. Li, K. Chen, C. Li, X. Zhang, L. An, J. Am. Ceram. Soc. 104 (2021)
1953–1958.
[435] V.E. Zhivulin, E.A. Trofimov, S.A. Gudkova, I.Y. Pashkeev, A.Y. Punda,
M. Gavrilyak, O.V. Zaitseva, S.V. Taskaev, F.V. Podgornov, M.A. Darwish, M.
A. Almessiere, Y. Slimani, A. Baykal, S.V. Trukhanov, A.V. Trukhanov, D.
A. Vinnik, Nanomaterials 11 (2021) 1014.
[436] Y. Zheng, M. Zou, W. Zhang, D. Yi, J. Lan, C.W. Nan, Y.H. Lin, J. Adv. Ceram. 10
(2021) 377–384.
[437] X. Zhang, Y. Li, C. Li, F. Yang, Z. Jiang, L. Xue, Z. Shao, Z. Zhao, M. Xie, S. Yu,
Mater. Des. 205 (2021), 109722.
[438] Z. Lun, B. Ouyang, D.H. Kwon, Y. Ha, E.E. Foley, T.Y. Huang, Z. Cai1, H. Kim,
M. Balasubramanian, Y. Sun, J. Huang, Y. Tian, H. Kim, B.D. McCloskey, W. Yang,
R.J. Clément, H. Ji, G. Ceder, Nat. Mater. 20 (2021) 214–221.
[439] W. Guo, S. Ma, L. Liu, Adv. Ceram. 38 (2017) 159–175.
[440] X. Wang, H. Xiang, X. Sun, J. Liu, F. Hou, Y. Zhou, J. Mater. Res. 29 (2014)
2673–2681.
[441] J.L. Braun, C.M. Rost, M. Lim, A. Giri, D.H. Olson, G.N. Kotsonis, G. Stan, D.
W. Brenner, J.P. Maria, P.E. Hopkins, Adv. Mater. 30 (2018), 1805004.
[442] J. Yang, X. Qian, W. Pan, R. Yang, Z. Li, Y. Han, M. Zhao, M. Huang, C. Wan, Adv.
Mater. 31 (2019), 1808222.
[443] V.F. Gorban, A.A. Andreev, A.M. Chikryzhov, M.V. Karpets, N.A. Krapivka, A.
V. Dolomanov, A.A. Ostroverkh, J. Superhard Mater. 41 (2019) 38–42.
[444] Z.M. Yang, K. Zhang, N. Qiu, H.B. Zhang, Y. Wang, J. Chen, Chinese Phys. B 28
(2019), 046201.
[445] G.N. Kotsonis, C.M. Rost, D.T. Harris, J.P. Maria, MRS Commun. 8 (2018)
1371–1377.
[446] A.J. Wright, C. Huang, M.J. Walock, A. Ghoshal, M. Murugan, J. Luo, J. Am.
Ceram. Soc. 104 (2021) 448–462.
[447] R. Liu, H. Chen, K. Zhao, Y. Qin, B. Jiang, T. Zhang, G. Sha, X. Shi, C. Uher,
W. Zhang, L. Chen, Adv. Mater. 29 (2017), 1702712.
[448] K. Chen, X. Pei, L. Tang, H. Cheng, Z. Li, C. Li, X. Zhang, L. An, J. Eur. Ceram. Soc.
38 (2018) 4161–4164.
[449] B. Liu, Y. Liu, C. Zhu, H. Xiang, H. Chen, L. Sun, Y. Gao, Y. Zhou, J. Mater. Sci.
Technol. 35 (2019) 833–851.
[450] M. Zhao, X. Ren, J. Yang, W. Pan, J. Am. Ceram. Soc. 99 (2016) 293–299.
[451] J.T.S. Irvine, A.J. Feighery, D.P. Fagg, S. Garcı́a-Martı́n, Solid State Ion. 136
(2000) 879–885.
[452] J.P. Goff, W. Hayes, S. Hull, M.T. Hutchings, K.N. Clausen, Phys. Rev. B 59 (1999)
14202.
[453] A. Bogicevic, C. Wolverton, G.M. Crosbie, E.B. Stechel, Phys. Rev. B 64 (2001),
014106.
[454] E.D. Wachsman, J. Eur. Ceram. Soc. 24 (2004) 1281–1285.
[455] J.F. Bisson, D. Fournier, M. Poulain, O. Lavigne, R. Mévrel, J. Am. Ceram. Soc. 83
(2000) 1993–1998.
[456] J. Zhu, X. Meng, J. Xu, P. Zhang, Z. Lou, M.J. Reece, F. Gao, J. Eur. Ceram. Soc. 41
(2021) 1052–1057.
[457] S.H. Albedwawi, A. AlJaberi, G.N. Haidemenopoulos, K. Polychronopoulou,
Mater. Des. 202 (2021), 109534.
[458] B. You, N. Jiang, M. Sheng, M.W. Bhushan, Y. Sun, ACS Catal. 6 (2016) 714–721.
[459] B. You, X. Liu, X. Liu, Y. Sun, ACS Catal. 7 (2017) 4564–4570.
[460] B. You, N. Jiang, M. Sheng, M.W. Bhushan, Y. Sun, ACS Catal. 6 (2016) 714–721.
[461] B. You, Y. Zhang, P. Yin, D.E. Jiang, Y. Sun, Nano Energy 48 (2018) 600–606.
[462] Y. Qiao, Y. Wang, H. Tian, M. Li, J. Jian, Y. Wei, Y. Tian, D.Y. Wang, Y. Pang,
X. Geng, X. Wang, Y. Zhao, H. Wang, N. Deng, M. Jian, Y. Zhang, R. Liang,
Y. Yang, T.L. Ren, ACS Nano 12 (2018) 8839–8846.
[463] Z. Liu, Y. Wang, R. Chen, C. Chen, H. Yang, J. Ma, Y. Li, S. Wang, J. Power Sources
403 (2018) 90–96.
[464] Z. Liu, C.L. Dong, Y.C. Huang, J. Cen, H. Yang, X. Chen, X. Tong, D. Su, Y. Wang,
S. Wang, J. Mater. Chem. 7 (2019) 14483–14488.
[465] D. Chen, C. Chen, Z.M. Baiyee, Z. Shao, F. Ciucci, Chem. Rev. 115 (2015)
9869–9921.
[466] H. Xu, Z. Zhang, J. Liu, C.L. Do-Thanh, H. Chen, S. Xu, Q. Lin, Y. Jiao, J. Wang,
Y. Wang, Y. Chen, S. Dai, Nat. Commun. 11 (2020) 3908.
[467] H. Chen, K. Jie, C.J. Jafta, Z. Yang, S. Yao, M. Liu, Z. Zhang, J. Liu, M. Chi, J. Fu,
S. Dai, Appl. Catal. B: Environ. 276 (2020), 119155.
[468] X. Ji, L.F. Nazar, J. Mater. Chem. 20 (2010) 9821–9826.
[469] A. Eftekhari, D.W. Kim, J. Mater. Chem. A 5 (2017) 17734–17776.
[470] Z. Sun, J. Zhang, L. Yin, G. Hu, R. Fang, H.M. Cheng, F. Li, Nat. Commun. 8
(2017) 14627.
[471] M.A. Pope, I.A. Aksay, Adv. Energy Mater. 5 (2015), 1500124.
S. Akrami et al.
[472] J.S. Kim, T.H. Hwang, B.G. Kim, J. Min, J.W. Choi, Adv. Funct. Mater. 24 (2014)
5359–5367.
[473] P.G. Bruce, L.J. Hardwick, K.M. Abraham, MRS Bull. 36 (2011) 506–512.
[474] J.Q. Huang, Q. Zhang, F. Wei, Energy Storage Mater. 1 (2015) 127–145.
[475] M.R. Busche, P. Adelhelm, H. Sommer, H. Schneider, K. Leitner, J. Janek,
J. Power Sources 259 (2014) 289–299.
[476] D. Liu, C. Zhang, G. Zhou, W. Lv, G. Ling, L. Zhi, Q.H. Yang, Adv. Sci. 5 (2018),
1700270.
[477] Y.V. Mikhaylik, J.R. Akridge, J. Electrochem. Soc. 151 (2004) A1969–A1976.
[478] H. Wang, W. Zhang, J. Xu, Z. Guo, Adv. Funct. Mater. 28 (2018), 1707520.
[479] Z.W. Zhang, H.J. Peng, M. Zhao, J.Q. Huang, Adv. Funct. Mater. 28 (2018),
1707536.
[480] R. Ponraj, A.G. Kannan, J.H. Ahn, D.W. Kim, ACS Appl. Mater. Interfaces 8 (2016)
4000–4006.
[481] Q. Pang, D. Kundu, M. Cuisinier, L.F. Nazar, Nat. Commun. 5 (2014) 4759.
[482] S.A. Ahad, P. Ragupathy, S. Ryu, H.W. Lee, D.K. Kim, Chem. Commun. 53 (2017)
8782–8785.
[483] X. Liang, A. Garsuch, L.F. Nazar, Angew. Chem. 127 (2015) 3979–3983.
[484] X. Ji, K.T. Lee, L.F. Nazar, Nat. Mater. 8 (2009) 500–506.
[485] H. Shao, F. Ai, W. Wang, H. Zhang, A. Wang, W. Feng, Y. Huang, J. Mater. Chem.
A 5 (2017) 19892–19900.
[486] Y. Liang, N. Deng, J. Ju, X. Zhou, J. Yan, C. Zhong, W. Kang, B. Cheng,
Electrochim. Acta 281 (2018) 257–265.
[487] R. Carter, B. Davis, L. Oakes, M.R. Maschmann, C.L. Pint, Nanoscale 9 (2017)
15018–15026.
[488] J. Guo, Y. Xu, C. Wang, Nano Lett. 11 (2011) 4288–4294.
[489] R. Carter, L. Oakes, N. Muralidharan, A.P. Cohn, A. Douglas, C.L. Pint, ACS Appl.
Mater. Interfaces 9 (2017) 7185–7192.
[490] Q. Sun, B. Xi, J.Y. Li, H. Mao, X. Ma, J. Liang, J. Feng, S. Xiong, Adv. Energy
Mater. 8 (2018), 1800595.
[491] Y. Zhang, Y. Zhao, A. Yermukhambetova, Z. Bakenov, P. Chen, J. Mater. Chem. A
1 (2013) 295–301.
[492] W. Li, J. Hicks-Garner, J. Wang, J. Liu, A.F. Gross, E. Sherman, J. Graetz, J.
J. Vajo, P. Liu, Chem. Mater. 26 (2014) 3403–3410.
[493] Q. Fan, W. Liu, Z. Weng, Y. Sun, H. Wang, J. Am. Chem. Soc. 137 (2015)
12946–12953.
[494] T. Nguyen, M. Boudard, L. Rapenne, M.J. Carmezim, M.F. Montemor, J. Mater.
Chem. 3 (2015) 10875–10882.
[495] X. Liu, J.Q. Huang, Q. Zhang, L. Mai, Adv. Mater. 29 (2017), 1601759.
[496] C. Mullens, M. Pikulski, S. Agachan, W. Gorski, J. Am. Chem. Soc. 125 (2003)
13602–13608.
[497] S.R. Mangisetti, B. Pari, M. Kamaraj, S. Ramaprabhu, ChemSusChem 11 (2018)
1664–1677.
[498] P.A. Deshpande, M.S. Hegde, G. Madras, AIChE J. 56 (2010) 1315–1324.
[499] R. Radhakrishnan, R.R. Willigan, Z. Dardas, T.H. Vanderspurt, AIChE J. 52 (2006)
1888–1894.
[500] R.J. Gorte, AIChE J. 56 (2010) 1126–1135.
[501] T. Bunluesin, R.J. Gorte, G.W. Graham, Appl. Catal. B: Environ. 15 (1998)
107–114.
[502] A. Kambolis, H. Matralis, A. Trovarelli, C. Papadopoulou, Appl. Catal. A Gen. 377
(2010) 16–26.
[503] T. Wang, F. Jiang, G. Liu, L. Zeng, Z.J. Zhao, J. Gong, AIChE J. 62 (2016)
4365–4376.
[504] E. Gomez, Z. Xie, J.G. Chen, AIChE J. 65 (2019), e16670.
[505] Y. Shu, J. Bao, S. Yang, X. Duan, P. Zhang, AIChE J. 67 (2021), e17046.
[506] M. Faraday, Philos. Trans. Biol. Sci. 129 (1839) 1–12.
[507] N.J. Dudney, J. Li, Science 347 (2015) 131–132.
[508] P. Poizot, S. Laruelle, S. Grugeon, L. Dupont, J.M. Tarascon, Nature 407 (2000)
496–499.
[509] D. Xiong, X. Li, Z. Bai, S. Lu, Small 14 (2018), 1703419.
[510] W. Liu, X. Li, D. Xiong, Y. Hao, J. Li, H. Kou, B. Yan, D. Li, S. Lu, A. Koo, K. Adair,
X. Sun, Nano Energy 44 (2018) 111–120.
[511] H. Wang, X. Yang, Q. Wu, Q. Zhang, H. Chen, H. Jing, J. Wang, S.B. Mi, A.
L. Rogach, C. Niu, ACS Nano 12 (2018) 3406–3416.
[512] S. Lim, J.H. Kim, Y. Yamada, H. Munakata, Y.S. Lee, S.S. Kim, K. Kanamura,
J. Power Sources 355 (2017) 164–170.
[513] M.V. Reddy, G. Prithvi, K.P. Loh, B.V.R. Chowdari, ACS Appl. Mater. Interfaces 6
(2014) 680–690.
[514] H. Zhang, G. Zhang, Z. Li, K. Qu, L. Wang, W. Zeng, Q. Zhang, H. Duan, J. Mater.
Chem. A 4 (2016) 10585–10592.
[515] Q. Zhang, J. Wang, D. Xu, Z. Wang, X. Li, K. Zhang, J. Mater. Chem. A 2 (2014)
3865–3874.
[516] Q. Zhang, D. Xu, X. Zhou, X. Wu, K. Zhang, Small 10 (2014) 935–943.
[517] F.X. Ma, H. Hu, H.B. Wu, C.Y. Xu, Z. Xu, L. Zhen, X.W. Lou, Adv. Mater. 27 (2015)
4097–4101.
[518] S.H. Lee, S.H. Yu, J.E. Lee, A. Jin, D.J. Lee, N. Lee, H. Jo, K. Shin, T.Y. Ahn, Y.
W. Kim, H. Shoe, Y.E. Sung, T. Hyeon, Nano Lett. 13 (2013) 4249–4256.
[519] B. Wang, H.B. Wu, L. Zhang, X.W. Lou, Angew. Chem. 125 (2013) 4259–4262.
[520] S. Petnikota, S.K. Marka, A. Banerjee, M.V. Reddy, V.V.S.S. Srikanth, B.V.
R. Chowdari, J. Power Sources 293 (2015) 253–263.
[521] J. Wang, H. Zhou, J. Nanda, P.V. Braun, Chem. Mater. 27 (2015) 2803–2811.
[522] L. Zhang, H.B. Wu, R. Xu, X.W. Lou, CrystEngComm 15 (2013) 9332–9335.
[523] E. Lokcu, C. Toparli, M. Anik, ACS Appl. Mater. Interfaces 12 (2020)
23860–23866.
[524] M. Kheradmandfard, H. Minouei, N. Tsvetkov, A.K. Vayghan, S.F. Kashani-
Bozorg, G. Kim, S.I. Hong, D.E. Kim, Mater. Chem. Phys. 262 (2021), 124265.
60
Materials Science & Engineering R 146 (2021) 100644
[525] D. Wang, S. Jiang, C. Duan, J. Mao, Y. Dong, K. Dong, Z. Wang, S. Luo, Y. Liu,
X. Qi, J. Alloys. Compd. 844 (2020), 156158.
[526] F. Tavani, M. Fracchia, N. Pianta, P. Ghigna, E. Quartarone, P. D’Angelo, Chem.
Phys. Lett. 760 (2020), 137968.
[527] J.C. Bachman, S. Muy, A. Grimaud, H.H. Chang, N. Pour, S.F. Lux, O. Paschos,
F. Maglia, S. Lupart, P. Lamp, L. Giordano, Y. Shao-Horn, Chem. Rev. 116 (2016)
140–162.
[528] J.W. Fergus, J. Power Sources 195 (2010) 4554–4569.
[529] H. Liu, G. Wang, J. Liu, S. Qiao, H. Ahn, J. Mater. Chem. 21 (2011) 3046–3052.
[530] C. Wang, Q. Li, F. Wang, G. Xia, R. Liu, D. Li, N. Li, J.S. Spendelow, G. Wu, ACS
Appl. Mater. Interfaces 6 (2014) 1243–1250.
[531] J.B. Goodenough, in: W.A. van Schalkwijk, B. Scrosati (Eds.), Advances in
Lithium-Ion Batteries, Springer, Boston, MA, USA, 2002, pp. 135–154.
[532] G.G. Amatucci, N. Pereira, J. Fluor. Chem. 128 (2007) 243–262.
[533] T.X. Nguyen, J. Patra, J.K. Chang, J.M. Ting, J. Mater. Chem. A 8 (2020)
18963–18973.
[534] J.R. Szczech, S. Jin, Energy Environ. Sci. 4 (2011) 56–72.
[535] V. Meunier, J. Kephart, C. Roland, J. Bernholc, Phys. Rev. Lett. 88 (2002),
075506.
[536] C.M. Schauerman, M.J. Ganter, G. Gaustad, C.W. Babbitt, R.P. Raffaelle, B.
J. Landi, J. Mater. Chem. 22 (2012) 12008–12015.
[537] K. Nishidate, M. Hasegawa, Phys. Rev. B 71 (2005), 245418.
[538] J. Zhao, A. Buldum, J. Han, J.P. Lu, Phys. Rev. Lett. 85 (2000) 1706.
[539] H. Fujimoto, K. Tokumitsu, A. Mabuchi, N. Chinnasamy, T. Kasuh, J. Power
Sources 195 (2010) 7452–7456.
[540] J. Yang, X.Y. Zhou, J. Li, Yl. Zou, J.J. Tang, Mater. Chem. Phys. 135 (2012)
445–450.
[541] C.A. Bridges, X.G. Sun, J. Zhao, M.P. Paranthaman, S. Dai, J. Phys. Chem. C 116
(2012) 7701–7711.
[542] Z. Wang, L. Zhou, X.W. Lou, Adv. Mater. 24 (2012) 1903–1911.
[543] J. Jiang, Y. Li, J. Liu, X. Huang, C. Yuan, X.W. Lou, Adv. Mater. 24 (2012)
5166–5180.
[544] P.P. Prosini, M. Carewska, S. Loreti, C. Minarini, S. Passerini, Int. J. Inorg. Mater.
2 (2000) 365–370.
[545] J. Wang, Y. Cui, Q. Wang, K. Wang, X. Huang, D. Stenzel, A. Sarkar, R. Azmi,
T. Bergfeldt, S.S. Bhattacharya, R. Kruk, H. Hahn, S. Schweidler, T. Brezesinski,
B. Breitung, Sci. Rep. 10 (2020) 18430.
[546] C. Zhao, F. Ding, Y. Lu, L. Chen, Y.S. Hu, Angew. Chem. 59 (2020) 264–269.
[547] C. Zhao, Y. Lu, L. Chen, Y.S. Hu, Nano Res. 12 (2019) 2018–2030.
[548] J. Wang, D. Stenzel, R. Azmi, S. Najib, K. Wang, J. Jeong, A. Sarkar, Q. Wang, P.
A. Sukkurji, T. Bergfeldt, M. Botros, J. Maibach, H. Hahn, T. Brezesinski,
B. Breitung, Electrochem 1 (2020) 60–74.
[549] M. Gazda, T. Miruszewski, D. Jaworski, A. Mielewczyk-Gryń , W. Skubida,
S. Wachowski, P. Winiarz, K. Dzierzgowski, M. Łapiń ski, I. Szpunar, E. Dzik, ACS
Mater. Lett. 2 (2020) 1315–1321.
[550] A. Bhattacharya, S.J. May, Annu. Rev. Mater. Res. 44 (2014) 65–90.
[551] K.J. Choi, M. Biegalski, Y.L. Li, A. Sharan, J. Schubert, R. Uecker, P. Reiche, Y.
B. Chen, X.Q. Pan, V. Gopalan, L.Q. Chen, D.G. Schlom, C.B. Eom, Science 306
(2004) 1005–1009.
[552] A. Sarkar, R. Kruk, H. Hahn, Dalton Trans. 50 (2021) 1973–1982.
[553] K. Simeonidis, M. Tziomaki, M. Angelakeris, C. Martinez-Boubeta, L. Balcells,
C. Monty, M. Mitrakas, G. Vourlias, N. Andritsos, EPJ Web Conf. 40 (2013)
08007.
[554] R.K. Singh, G.P. Kothiyal, A. Srinivasan, J. Non-Cryst. Solids 354 (2008)
3166–3170.
[555] R.K. Singh, G.P. Kothiyal, A. Srinivasan, Solid State Commun. 146 (2008) 25–29.
[556] R.T. Smith, F.S. Welsh, J. Appl. Phys. 42 (1971) 2219–2230.
[557] Y. Cho, K. Yamanouchi, J. Appl. Phys. 61 (1987) 875–887.
[558] J. Hladik (Ed.), Physics of Electrolytes, Vol. 1, Academic Press, London, New
York, 1972.
[559] X.J. Chen, K.A. Khor, S.H. Chan, L.G. Yu, Mater. Sci. Eng. A 335 (2002) 246–252.
[560] C.H. Tsau, Z.Y. Hwang, S.K. Chen, Adv. Mater. Sci. Eng. Int. J. 2015 (2015),
353140.
[561] K. Edalati, M. Arimura, Y. Ikoma, T. Daio, M. Miyata, D.J. Smith, Z. Horita, Mater.
Res. Lett. 3 (2015) 216–221.
[562] Y. Zou, H. Ma, R. Spolenak, Nat. Commun. 6 (2015) 7748.
[563] B. Cheng, Q. Li, H. Zhang, R. Liu, B. Liu, Z. Yao, T. Cui, J. Liu, Z. Liu, B. Sundqvist,
B. Liu, Phys. Rev. B 93 (2016), 184109.
[564] R.S. McWilliams, D.K. Spaulding, J.H. Eggert, P.M. Celliers, D.G. Hicks, R.
F. Smith, G.W. Collins, R. Jeanloz, Science 338 (2012) 1330–1333.
[565] A. Sarkar, B. Eggert, L. Velasco, X. Mu, J. Lill, K. Ollefs, S.S. Bhattacharya,
H. Wende, R. Kruk, R.A. Brand, H. Hahn, APL Mater. 8 (2020), 051111.
[566] J. de Wild, J.K. Rath, A. Meijerink, W.G.J.H.M. van Sark, R.E.I. Schropp, Sol.
Energy Mater. Sol. Cells 94 (2010) 2395–2398.
[567] M. Rüdiger, S. Fischer, J. Frank, A. Ivaturi, B.S. Richards, K.W. Krämer,
M. Hermle, J.C. Goldschmidt, Sol. Energy Mater. Sol. Cells 128 (2014) 57–68.
[568] S. Fischer, B. Fröhlich, H. Steinkemper, K.W. Krämer, J.C. Goldschmidt, Sol.
Energy Mater. Sol. Cells 122 (2014) 197–207.
[569] L. Qiu, Y. Yang, G. Dong, D. Xia, M. Li, X. Fan, R. Fan, Appl. Surf. Sci. 448 (2018)
145–153.
[570] C. Yen-Chi, H. Woan-Yu, C. Teng-Ming, J. Rare Earths 29 (2011) 907–910.
[571] G. Shao, C. Lou, D. Xiao, J. Lumin. 157 (2015) 344–348.
[572] V. Kumar, S.K. Swami, A. Kumar, O.M. Ntwaeaborwa, V. Dutta, H.C. Swart,
J. Colloid Interface Sci. 484 (2016) 24–32.
[573] X. Huang, S. Han, W. Huang, X. Liu, Chem. Soc. Rev. 42 (2013) 173–201.
[574] M. Hanioka, Y. Furukawa, H. Samata, Optik 180 (2019) 1043–1048.
S. Akrami et al.
[575] A.C. Vlasveld, S.G. Harris, E.D. Doyle, D.B. Lewis, W.D. Munz, Surf. Coat.
Technol. 149 (2002) 217–223.
[576] W.D. Münz, J. Vacuum Sci. Technol. A 4 (1986) 2717–2725.
[577] T.T.H. Pham, E.L. Bourhis, P. Goudeau, P. Guérin, Mater. Sci. Forum 695 (2011)
182–185.
[578] H. Willmann, P.H. Mayrhofer, P.O.Å. Persson, A.E. Reiter, L. Hultman,
C. Mitterer, Scr. Mater. 54 (2006) 1847–1851.
[579] S.A. Glatz, C.M. Koller, H. Bolvardi, S. Kolozsvári, H. Riedl, P.H. Mayrhofer, Surf.
Coat. Technol. 311 (2017) 330–336.
[580] H. Asanuma, F.F. Klimashin, P. Polcik, S. Kolozsvári, H. Riedl, P.H. Mayrhofer,
Thin Solid Films 688 (2019), 137239.
[581] H. Asanuma, F.F. Klimashin, P. Polcik, S. Kolozsvári, H. Riedl, P.H. Mayrhofer,
Surf. Coat. Technol. 372 (2019) 26–33.
[582] M. Wittmer, J. Noser, H. Melchior, J. Appl. Phys. 52 (1981) 6659–6664.
[583] M. Zhou, Y. Makino, M. Nose, K. Nogi, Thin Solid Films 339 (1999) 203–208.
[584] S. PalDey, S.C. Deevi, Mater. Sci. Eng. A 342 (2003) 58–79.
[585] L.A. Donohue, I.J. Smith, W.D. Münz, I. Petrov, J.E. Greene, Surf. Coat. Technol.
94-95 (1997) 226–231.
[586] Y. Zhang, W.M. Guo, Z.B. Jiang, Q.Q. Zhu, S.K. Sun, Y. You, K. Plucknett, H.T. Lin,
Scr. Mater. 164 (2019) 135–139.
[587] M.H. Tsai, C.W. Wang, C.H. Lai, J.W. Yeh, J.Y. Gan, Appl. Phys. Lett. 92 (2008),
052109.
[588] C.W. Tsai, S.W. Lai, K.H. Cheng, M.H. Tsai, A. Davison, C.H. Tsau, J.W. Yeh, Thin
Solid Films 520 (2012) 2613–2618.
[589] A.D. Pogrebnjak, J. Nanomater. 2013 (2013), 780125.
[590] A.D. Pogrebnjak, I.V. Yakushchenko, G. Abadias, P. Chartier, O.V. Bondar, V.
M. Beresnev, Y. Takeda, O.V. Sobol, K. Oyoshi, A.A. Andreyev, B.A. Mukushev,
J. Superhard Mater. 35 (2013) 356–368.
[591] S.Y. Chang, Y.C. Huang, C.E. Li, H.F. Hsu, J.W. Yeh, S.J. Lin, JOM 65 (2013)
1790–1796.
[592] A.D. Pogrebnjak, A.A. Bagdasaryan, I.V. Yakushchenko, V.M. Beresnev, Russ.
Chem. Rev. 83 (2014) 1027.
[593] A. Bagdasaryan, P. Konarski, M. Misnik, F. Komarov, The distribution analysis for
elements in depth of nitride coating based on high-entropy Ti-Hf-V-Nb-Zr alloy,
in: Proceedings of the 24th International Crimean Conference Microwave &
Telecommunication Technology, IEEE, Sevastopol, Ukraine, 2014, pp. 779–780.
[594] V.F. Gorban, I.M. Zakiev, G.F. Sarzhan, J. Frict. Wear 37 (2016) 263–267.
[595] A.A. Vereschaka, B.Y. Mokritskii, N.N. Sitnikov, G.V. Oganyan, A.Y. Aksenenko,
J. Nano Res. 45 (2017) 110–123.
[596] Y.O. Tleukenov, S.V. Plotnikov, A.D. Pogrebnjak, N.K. Erdybaeva, A.
B. Manapbayeva, Rec. Contr. Phys. 60 (2018) 62–71.
[597] O.V. Sobol, O. Dur, А.A. Postelnyk, Z.V. Kraievska, Funct. Mater. 26 (2019)
310–318.
[598] Y.S. Kim, H.J. Park, K.S. Lim, S.H. Hong, K.B. Kim, Coatings 10 (2020) 10.
[599] J.J. Wang, F.Y. Ouyang, Corros. Sci. 187 (2021), 109467.
[600] Y. Xu, G. Li, G. Li, F. Gao, Y. Xia, Appl. Surf. Sci. 564 (2021), 150417.
[601] X. Lu, C. Zhang, C. Wang, X. Cao, R. Ma, X. Sui, J. Hao, W. Liu, Appl. Surf. Sci. 557
(2021), 149813.
[602] W. Yu, W. Li, P. Liu, K. Zhang, F. Ma, X. Chen, R. Feng, P.K. Liaw, Mater. Des. 203
(2021), 109553.
[603] A. Xia, R. Dedoncker, O. Glushko, M.J. Cordill, D. Depla, R. Franz, J. Alloys.
Compd. 850 (2021), 156740.
[604] S.K. Bachani, C.J. Wang, B.S. Lou, L.C. Chang, J.W. Lee, J. Alloys. Compd. 873
(2021), 159605.
[605] H. Zaid, K. Tanaka, C.V. Ciobanu, J.M. Yang, S. Kodambaka, H. Kindlund, Scr.
Mater. 197 (2021), 113813.
[606] W.H. Kao, Y.L. Su, J.H. Horng, C.M. Wu, Surf. Coat. Technol. 405 (2021), 126539.
[607] W. Xu, M. Liao, X. Liu, L. Ji, P. Ju, H. Li, H. Zhou, J. Chen, Ceram. Int. 47 (2021)
24752–24759.
[608] L.W. Lan, H.J. Yang, R.P. Guo, X.J. Wang, M. Zhang, P.K. Liaw, J.W. Qiao, Mater.
Chem. Phys. 270 (2021), 124800.
[609] M.H. Hsieh, M.H. Tsai, W.J. Shen, J.W. Yeh, Surf. Coat. Technol. 221 (2013)
118–123.
[610] P.K. Huang, J.W. Yeh, Surf. Coat. Technol. 203 (2009) 1891–1896.
[611] P. Cui, W. Li, P. Liu, K. Zhang, F. Ma, X. Chen, R. Feng, P.K. Liaw, J. Alloys.
Compd. 834 (2020), 155063.
[612] Y.C. Lin, S.Y. Hsu, R.W. Song, W.L. Lo, Y.T. Lai, S.Y. Tsai, J.G. Duh, Surf. Coat.
Technol. 403 (2020), 126417.
[613] W.J. Shen, M.H. Tsai, J.W. Yeh, Coatings 5 (2015) 312–325.
[614] P.K. Huang, J.W. Yeh, Scr. Mater. 62 (2010) 105–108.
[615] A.D. Pogrebnjak, I.V. Yakushchenko, A.A. Bagdasaryan, O.V. Bondar, R. Krause-
Rehberg, G. Abadias, P. Chartier, K. Oyoshi, Y. Takeda, V.M. Beresnev, O.V. sobol,
Mater. Chem. Phys. 147 (2014) 1079–1091.
[616] D. Moskovskikh, S. Vorotilo, V. Buinevich, A. Sedegov, K. Kuskov, A. Khort,
C. Shuck, M. Zhukovskyi, A. Mukasyan, Sci. Rep. 10 (2020) 19874.
[617] S.A. Firstov, V.F. Gorban, N.I. Danilenko, M.V. Karpets, A.A. Andreev, E.
S. Makarenko, Powder Metall. Met. Ceram. 52 (2014) 560–566.
[618] A.D. Pogrebnjak, A.A. Bagdasaryan, V.M. Beresnev, A.I. Kupchishin, S.
V. Plotnikov, Y.O. Kravchenko, High Temp. Mater. Process. 21 (2017) 261–275.
[619] U.S. Nyemchenko, V.J. Novikov, V.A. Stolbovoy, V.M. Beresnev, O.V. Sobol,
Voprosy Atomnoj Nauki i Tekhniki 46 (2015) 139–144.
[620] A. Bagdasaryan, A. Pogrebnjak, A. Pshyk, E. Coy, V. Beresnev, Synthesis and
characterization of nitride multilayerd coatings based on refractory metals, in:
Proceedings of the IEEE 7th International Conference Nanomaterials: Application
& Properties (NAP), IEEE, Odessa, UKraine, 2017, pp. 02NTF37-1–02NTF37-5.
61
Materials Science & Engineering R 146 (2021) 100644
[621] W.J. Shen, M.H. Tsai, Y.S. Chang, J.W. Yeh, Thin Solid Films 520 (2012)
6183–6188.
[622] O.V. Sobol, A.A. Andreev, V.F. Gorban, A. Meylekhov, А.A. Postelnyk,
V. Stolbovoy, A.V. Zvyagolskiy, J. Nano- Electron. Phys. 10 (2018) 06030.
[623] M.H. Tsai, C.H. Lai, J.W. Yeh, J.Y. Gan, J. Phys. D Appl. Phys. 41 (2008), 235402.
[624] C.H. Chang, P.W. Li, Q.Q. Wu, M.H. Wang, C.C. Sung, C.Y. Hsu, Mater. Technol.
34 (2019) 343–349.
[625] Z.C. Chang, Mater. Chem. Phys. 220 (2018) 98–110.
[626] Q.W. Xing, S.Q. Xia, X.H. Yan, Y. Zhang, J. Mater. Res. 33 (2018) 3347–3354.
[627] J.J. Wang, S.Y. Chang, F.Y. Ouyang, Surf. Coat. Technol. 393 (2020), 125796.
[628] C.H. Lai, M.H. Tsai, S.J. Lin, J.W. Yeh, Surf. Coat. Technol. 201 (2007)
6993–6998.
[629] C.H. Lai, S.J. Lin, J.W. Yeh, S.Y. Chang, Surf. Coat. Technol. 201 (2006)
3275–3280.
[630] K. Johansson, L. Riekehr, S. Fritze, E. Lewin, Surf. Coat. Technol. 349 (2018)
529–539.
[631] P.K. Huang, J.W. Yeh, Thin Solid Films 518 (2009) 180–184.
[632] K. von Fieandt, E.M. Paschalidou, A. Srinath, P. Soucek, L. Riekehr, L. Nyholm,
E. Lewin, Thin Solid Films 693 (2020), 137685.
[633] A. Nishimoto, T. Fukube, T. Maruyama, Surf. Coat. Technol. 376 (2019) 52–58.
[634] O.F. Dippo, N. Mesgarzadeh, T.J. Harrington, G.D. Schrader, K.S. Vecchio, Sci.
Rep. 10 (2020) 21288.
[635] N.A. Khan, B. Akhavan, C. Zhou, H. Zhou, L. Chang, Y. Wang, Y. Liu, M.M. Bilek,
Z. Liu, Surf. Coat. Technol. 402 (2020), 126327.
[636] O.V. Sobol, A.A. Andreev, V.F. Gorban, H.O. Postelnyk, V.A. Stolbovoy, A.
V. Zvyagolsky, A.V. Dolomanov, Z.V. Kraievska, Probl. At. Sci. Technol. 120
(2019) 127–135.
[637] A.A. Bagdasaryan, A.V. Pshyk, L.E. Coy, M. Kempiński, A.D. Pogrebnjak, V.
M. Beresnev, S. Jurga, Mater. Lett. 229 (2018) 364–367.
[638] R. Hahn, A. Kirnbauer, M. Bartosik, S. Kolozsvári, P.H. Mayrhofer, Mater. Lett.
251 (2019) 238–240.
[639] H.T. Hsueh, W.J. Shen, M.H. Tsai, J.W. Yeh, Surf. Coat. Technol. 206 (2012)
4106–4112.
[640] W.J. Shen, M.H. Tsai, K.Y. Tsai, C.C. Juan, C.W. Tsai, J.W. Yeh, Y.S. Chang,
J. Electrochem. Soc. 160 (2013) C531.
[641] Y. Massiani, A. Medjahed, P. Gravier, L. Argème, L. Fedrizzi, Thin Solid Films 191
(1990) 305–316.
[642] Y. Massiani, J. Crousier, L. Fedrizzi, A. Cavalleri, P.L. Bonora, Surf. Coat. Technol.
33 (1987) 309–317.
[643] I. Milošev, H.H. Strehblow, B. Navinšek, Thin Solid Films 303 (1997) 246–254.
[644] U.K. Wiiala, I.M. Penttinen, A.S. Korhonen, J. Aromaa, E. Ristolainen, Surf. Coat.
Technol. 41 (1990) 191–204.
[645] J. Piippo, B. Elsener, H. Böhni, Surf. Coat. Technol. 61 (1993) 43–46.
[646] P.C. Andricacos, C. Uzoh, J.O. Dukovic, J. Horkans, H. Deligianni, IBM J. Res.
Dev. 42 (1998) 567–574.
[647] R. Rosenberg, D.C. Edelstein, C.K. Hu, K.P. Rodbell, Annu. Rev. Mater. Sci. 30
(2000) 229–262.
[648] Y. Wang, C.H. Zhao, F. Cao, D.W. Yang, Mater. Lett. 62 (2008) 3761–3763.
[649] Y. Wang, X. Chen, W. Ma, Y. Shang, Z. Lei, F. Xiang, Appl. Surf. Sci. 396 (2017)
333–338.
[650] S. Sharma, M. Kumar, S. Rani, D. Kumar, C.C. Tripathi, Mater. Sci. Semicond.
Process. 48 (2016) 1–8.
[651] A. Kumar, M. Kumar, D. Kumar, Appl. Surf. Sci. 258 (2012) 7962–7967.
[652] A. Cros, M.O. Aboelfotoh, K.N. Tu, J. Appl. Phys. 67 (1990) 3328–3336.
[653] L. Arnaud, T. Berger, G. Reimbold, J. Appl. Phys. 93 (2003) 192–204.
[654] E.G. Liniger, C.K. Hu, L.M. Gignac, A. Simon, J. Appl. Phys. 93 (2003)
9576–9582.
[655] K. Wetzig, C.M. Schneider (Eds.), Metal Based Thin Films for Electronics, WILEY-
VCH Verlag GmbH & Co. KGaA, Weinheim, 2004.
[656] S.Y. Chang, M.K. Chen, D.S. Chen, J. Electrochem. Soc. 156 (2009) G37.
[657] X. Lu, T. Liu, T. Zhai, G. Wang, M. Yu, S. Xie, Y. Ling, C. Liang, Y. Tong, Y. Li, Adv.
Energy Mater. 4 (2014), 1300994.
[658] L. Zhang, C.M.B. Holt, E.J. Luber, B.C. Olsen, H. Wang, M. Danaie, X. Cui, X. Tan,
V.W. Lui, W.P. Kalisvaart, D. Mitlin, J. Phys. Chem. C 115 (2011) 24381–24393.
[659] C.Y. He, X.L. Qiu, D.M. Yu, S.S. Zhao, H.X. Guo, G. Liu, X.H. Gao, J. Materiomics 7
(2021) 460–469.
[660] H.X. Guo, D.M. Yu, C.Y. He, X.L. Qiu, S.S. Zhao, G. Liu, X.H. Gao, J. Surf.
Interfaces Mater. 24 (2021), 101062.
[661] S.S. Zhao, X.L. Qiu, C.Y. He, D.M. Yu, G. Liu, X.H. Gao, ACS Appl. Nano Mater. 4
(2021) 4504–4512.
[662] C.Y. He, X.H. Gao, X.L. Qiu, D.M. Yu, H.X. Guo, G. Liu, Sol. RRL 5 (2021),
2000790.
[663] C.Y. He, X.H. Gao, D.M. Yu, X.L. Qiu, H.X. Guo, G. Liu, J. Mater. Chem. A Mater.
Energy Sustain. 9 (2021) 6413.
[664] J. Dusza, P. Švec, V. Girman, R. Sedlák, E.G. Castle, T. Csanádi, A. Kovalčíková,
M.J. Reece, J. Eur. Ceram. Soc. 38 (2018) 4303–4307.
[665] A.S. Rogachev, A.N. Gryadunov, N.A. Kochetov, A.S. Schukin, F. Baras,
O. Politano, Int. J. Self-Propag. High-Temp. Synth. 28 (2019) 196–198.
[666] H. Zhang, F. Akhtar, Entropy 21 (2019) 474.
[667] N. Gao, D.H. Lu, Y.Y. Zhao, X.W. Liu, G.H. Liu, Y. Wu, G. Liu, Z.T. Fan, Z. Lu, E.
P. George, J. Alloys. Compd. 792 (2019) 1028–1035.
[668] L. Feng, W.G. Fahrenholtz, G.E. Hilmas, Y. Zhou, Scr. Mater. 162 (2019) 90–93.
[669] X. Han, V. Girman, R. Sedlak, J. Dusza, E.G. Castle, Y. Wang, M. Reece, C. Zhang,
J. Eur. Ceram. Soc. 40 (2020) 2709–2715.
[670] M. Biesuz, T.G. Saunders, K. Chen, M. Bortolotti, M. Salvo, S. Grasso, M.J. Reece,
J. Eur. Ceram. Soc. 40 (2020) 2699–2708.
S. Akrami et al.
[671] E. Chicardi, C. García-Garrido, F.J. Gotor, Ceram. Int. 45 (2019) 21858–21863.
[672] A. Sedegov, S. Vorotilo, V. Tsybulin, K. Kuskov, D. Moscovskikh, IOP Conf. Ser.:
Mater. Sci. Eng. 558 (2019), 012043.
[673] T. Csanádi, E. Castle, M.J. Reece, J. Dusza, Sci. Rep. 9 (2019) 10200.
[674] T. Csanádi, M. Vojtko, Z. Dankházi, M.J. Reece, J. Dusza, J. Eur. Ceram. Soc. 40
(2020) 4774–4782.
[675] Y. He, C. Peng, S. Xin, K. Li, S. Liang, X. Lu, N. Kang, H. Xue, X. Shen, T. Shen,
J. Mater. Sci. 55 (2020) 6754–6760.
[676] B. Du, H. Liu, Y. Chu, J. Am. Ceram. Soc. 103 (2020) 4063–4068.
[677] S.S. Hwang, A.L. Vasiliev, N.P. Padture, Mater. Sci. Eng. A 464 (2007) 216–224.
[678] G.J. Zhang, Z.Y. Deng, N. Kondo, J.F. Yang, T. Ohji, J. Am. Ceram. Soc. 83 (2000)
2330–2332.
[679] M. Gasch, D. Ellerby, E. Irby, S. Beckman, M. Gusman, S. Johnson, J. Mater. Sci.
39 (2004) 5925–5937.
[680] E. Sani, L. Mercatelli, D. Fontani, J.L. Sans, D. Sciti, J. Renew. Sustain. Energy 3
(2011), 063107.
[681] J.X. Liu, Y.M. Kan, G.J. Zhang, J. Am. Ceram. Soc. 93 (2010) 370–373.
[682] K. Wang, L. Chen, C. Xu, W. Zhang, Z. Liu, Y. Wang, J. Ouyang, X. Zhang, Y. Fu,
Y. Zhou, J. Mater. Sci. Technol. 39 (2020) 99–105.
[683] D. Liu, Y. Gao, J. Liu, K. Li, F. Liu, Y. Wang, L. An, J. Eur. Ceram. Soc. 36 (2016)
2051–2055.
[684] P.F. Becher, G.C. Wei, J. Am. Ceram. Soc. 67 (1984) C-267–C-269.
[685] A.L. Chamberlain, W.G. Fahrenholtz, G.E. Hilmas, D.T. Ellerby, J. Am. Ceram.
Soc. 87 (2004) 1170–1172.
[686] E. Castle, T. Csanádi, S. Grasso, J. Dusza, M. Reece, Sci. Rep. 8 (2018) 8609.
[687] D. Demirskyi, H. Borodianska, Ts. Suzuki, Y. Sakka, K. Yoshimi, O. Vasylkiv, Scr.
Mater. 164 (2019) 12–16.
[688] B. Ye, Y. Chu, K. Huang, D. Liu, J. Am. Ceram. Soc. 102 (2019) 919–923.
[689] P. Malinovskis, S. Fritze, L. Riekehr, L. von Fieandt, J. Cedervall, D. Rehnlund,
L. Nyholm, E. Lewin, U. Jansson, Materi. Des. 149 (2018) 51–62.
[690] V. Braic, A. Vladescu, M. Balaceanu, C.R. Luculescu, M. Braic, Surf. Coat. Technol.
211 (2012) 117–121.
[691] B. Ye, T. Wen, K. Huang, C.Z. Wang, Y. Chu, J. Am. Ceram. Soc. 102 (2019)
4344–4352.
[692] V. Braic, M. Balaceanu, M. Braic, A. Vladescu, S. Panseri, A. Russo, J. Mech.
Behav. Biomed. Mater. 10 (2012) 197–205.
[693] Y. Li, J. Lu, M. Li, K. Chang, X. Zha, Y. Zhang, K. Chen, P.O.A. Persson,
L. Hultman, P. Eklund, S. Du, J.S. Francisco, Z. Chai, Z. Huang, Q. Huang, Proc.
Natl. Acad. Sci. U.S.A. 117 (2020) 820–825.
[694] Q.Q. Wei, X.D. Xu, G.M. Li, G.Q. Luo, J. Zhang, Q. Shen b, C.L. Wu, Scr. Mater.
200 (2021), 113909.
[695] S. Guan, H. Liang, Q. Wang, L. Tan, F. Peng, Inorg. Chem. 60 (2021) 3807–3813.
̌
[696] P. Solcová, M. Nižň anský , J. Schulz, P. Brázda, P. Ecorchard, M. Vilémová,
V. Tyrpekl, Inorg. Chem. 60 (2021) 7617–7621.
[697] M.D. Hossain, T. Borman, A. Kumar, X. Chen, A. Khosravani, S.R. Kalidindi, E.
A. Paisley, M. Esters, C. Oses, C. Toher, S. Curtarolo, J.M. LeBeau, D. Brenner, J.
P. Maria, Acta Mater. 215 (2021), 117051.
[698] K. Sun, Z. Yang, R. Mu, S. Niu, Y. Wang, D. Wang, J. Eur. Ceram. Soc. 41 (2021)
3196–3206.
[699] X.F. Wei, J.X. Liu, W. Bao, Y. Qin, F. Li, Y. Liang, F. Xu, G.J. Zhang, J. Eur. Ceram.
Soc. 41 (2021) 4747–4754.
[700] J. Wang, H. Zhang, X. Yu, L. Wang, W. Huang, Z. Lu, Surf. Coat. Technol. 421
(2021), 127468.
[701] W.H. Kao, Y.L. Su, J.H. Horng, W.C. Wu, Mater. Chem. Phys. 268 (2021), 124741.
[702] J. Pötschke, M. Dahal, A. Vornberger, M. Herrmann, A. Michaelis, Metals 11
(2021) 271.
[703] J. Dusza, T. Csan´adi, D. Medveˇd, R. Sedl´ak, M. Vojtko, M. Ivor, H. Ünsal,
P. Tatarko, M. Tatarkov´a, P. ˇSajgalík, J. Eur. Ceram. Soc. 41 (2021) 5417–5426.
[704] K. Vasanthakumar, G. Revathi, S. Ariharan, S.R. Bakshi, J. Eur. Ceram. Soc. 41
(2021) 6756–6762.
[705] H. Wang, X. Han, W. Liu, Y. Wang, Ceram. Int. 47 (2021) 10848–10854.
[706] Z. Li, Z. Wang, Z. Wu, B. Xu, S. Zhao, W. Zhang, N. Lin, Ceram. Int. 47 (2021)
14341–14347.
[707] J. Potschke, M. Dahal, M. Herrmann, A. Vornberger, B. Matthey, A. Michaelis,
J. Mater. Sci. 56 (2021) 11237–11247.
[708] D. Yu, J. Yin, B. Zhang, X. Liu, M.J. Reece, W. Liu, Z. Huang, J. Eur. Ceram. Soc.
41 (2021) 3823–3831.
[709] Q. Sun, H. Tan, S. Zhu, Z. Zhu, L. Wang, J. Cheng, J. Yang, Tribol. Int. 157 (2021),
106883.
[710] D.G. Sangiovanni, W. Mellor, T. Harrington, K. Kaufmann, K. Vecchio, Mater. Des.
209 (2021), 109932.
[711] F. Cai, D. Ni, B. Chen, L. Ye, Y. Sun, J. Lu, X. Zou, H. Zhou, P. He, T. Zhao,
S. Dong, J. Eur. Ceram. Soc. 41 (2021) 5863–5871.
[712] K. Lu, J.X. Liu, X.F. Wei, W. Bao, Y. Wu, F. Li, F. Xu, G.J. Zhang, J. Eur. Ceram.
Soc. 40 (2020) 1839–1847.
[713] F. Wang, X. Zhang, X. Yan, Y. Lu, M. Nastasi, Y. Chen, B. Cui, J. Am. Ceram. Soc.
103 (2020) 4463–4472.
[714] W.H. Kan, Y. Zhang, X. Tang, T. Lucey, G. Proust, Y. Gan, J. Cairney, Materialia 9
(2020), 100540.
[715] D. Liu, A. Zhang, J. Jia, J. Meng, B. Su, J. Eur. Ceram. Soc. 40 (2020) 2746–2751.
62
Materials Science & Engineering R 146 (2021) 100644
[716] C. Peng, H. Tang, Y. He, X. Lu, P. Jia, G. Liu, Y. Zhao, M. Wang, J. Mater. Sci.
Technol. 51 (2020) 161–166.
[717] L. Feng, W.T. Chen, W.G. Fahrenholtz, G.E. Hilmas, J. Am. Ceram. Soc. 104
(2021) 419–427.
[718] Y. Wang, T. Csanádi, H. Zhang, J. Dusza, M.J. Reece, R.Z. Zhang, Adv. Theory
Simul. 3 (2020), 2000111.
[719] M. Braic, M. Balaceanu, A. Vladescu, C.N. Zoita, V. Braic, Appl. Surf. Sci. 284
(2013) 671–678.
[720] V. Braic, A.C. Parau, I. Pana, M. Braic, M. Balaceanu, Surf. Coat. Technol. 58
(2014) 996–1005.
[721] K. Upadhya, J.M. Yang, W.P. Hoffman, Am. Ceram. Soc. Bull 76 (1997) 51–56.
[722] H. Chen, H. Xiang, F.Z. Dai, J. Liu, Y. Lei, J. Zhang, Y. Zhou, J. Mater. Sci.
Technol. 35 (2019) 1700–1705.
[723] C.M. Rost, T. Borman, M.D. Hossain, M. Lim, K.F. Quiambao-Tomko, J.A. Tomko,
D.W. Brenner, J.P. Maria, P.E. Hopkins, Acta Mater. 196 (2020) 231–239.
[724] H. Cheng, H.Y. Wang, Y.C. Xie, Q.H. Tang, P.Q. Dai, Mater. Sci. Technol. 33
(2017) 2032–2039.
[725] C. Peng, H. Tang, Y. He, X. Lu, P. Jia, G. Liu, Y. Zhao, M. Wang, J. Mater. Sci.
Technol. 51 (2020) 161–166.
[726] J. Zhou, J. Zhang, F. Zhang, B. Niu, L. Lei, W. Wang, Ceram. Int. 44 (2018)
22014–22018.
[727] V.K. Balla, S. Bose, N.M. Davies, A. Bandyopadhyay, JOM 62 (7) (2010) 61–64.
[728] J. Probst, U. Gbureck, R. Thull, Surf. Coat. Technol. 148 (2001) 226–233.
[729] M. Brama, N. Rhodes, J. Hunt, A. Ricci, R. Teghil, S. Migliaccio, C.D. Rocca,
S. Leccisotti, A. Lioi, M. Scandurra, G. DeMaria, D. Ferro, F. Pu, G. Panzini,
L. Politi, R. Scandurra, Biomaterials 28 (2007) 595–608.
[730] C.L. Chu, H.L. Ji, L.H. Yin, Y.P. Pu, P.H. Lin, P.K. Chu, Mater. Sci. Eng. C 31
(2011) 423–427.
[731] A.P. Serro, C. Completo, R. Colaço, F. dos Santos, C.L. da Silva, J.M.S. Cabral,
H. Araújo, E. Pires, B. Saramago, Surf. Coat. Technol. 203 (2009) 3701–3707.
[732] C.M. Cotrut, V. Braic, M. Balaceanu, I. Titorencu, M. Braic, A.C. Parau, Thin Solid
Films 538 (2013) 48–55.
[733] A. Vladescu, A. Kiss, A. Popescu, M. Braic, M. Balaceanu, V. Braic, I. Tudor,
C. Logofatu, C.C. Negrila, R. Rapeanu, J. Nanosci. Nanotechnol. 8 (2008)
717–721.
[734] S. Vepřek, Surf. Coat. Technol. 97 (1997) 15–22.
[735] U. Jansson, E. Lewin, Thin Solid Films 536 (2013) 1–24.
[736] S. Santavirta, M. Takagi, L. Nordsletten, A. Anttila, R. Lappalainen, Y.
T. Konttinen, Arch. Orthop. Trauma. Surg. 118 (1998) 89–91.
[737] D.V. Shtansky, N.A. Gloushankova, A.N. Sheveiko, P.V. Kiryukhantsev-Korneev, I.
A. Bashkova, B.N. Mavrin, S.G. Ignatov, S.Y. Filippovich, C. Rojas, Surf. Coat.
Technol. 205 (2010) 728–739.
[738] Y. Zhou, B. Zhao, H. Chen, H. Xiang, F.Z. Dai, S. Wu, W. Xu, J. Mater. Sci.
Technol. 74 (2021) 105–118.
[739] L. Silvestroni, S. Guicciardi, C. Melandri, D. Sciti, J. Eur. Ceram. Soc. 32 (2012)
97–105.
[740] J. Yang, M.X. Wang, Y.B. Kang, D.J. Li, Appl. Surf. Sci. 253 (2007) 5302–5305.
[741] W.G. Fahrenholtz, J. Am. Ceram. Soc. 90 (2007) 143–148.
[742] R. Licheri, R. Orru, C. Musa, G. Cao, ACS Appl. Mater. Interfaces 2 (2010)
2206–2212.
[743] B. Ye, C. Fan, Y. Han, M. Ma, Y. Chu, J. Am. Ceram. Soc. 103 (2020) 4738–4741.
[744] J.X. Liu, X.Q. Shen, Y. Wu, F. Li, Y. Liang, G.J. Zhang, J. Adv. Ceram. 9 (2020)
503–510.
[745] F. Monteverde, F. Saraga, M. Gaboardi, J. Eur. Ceram. Soc. 40 (2020) 3807–3814.
[746] S. Failla, P. Galizia, S. Fu, S. Grasso, D. Sciti, J. Eur. Ceram. Soc. 40 (2020)
588–593.
[747] H. Chen, Z. Zhao, H. Xiang, F.Z. Dai, J. Zhang, S. Wang, J. Liu, Y. Zhou, J. Mater.
Sci. Technol. 38 (2020) 80–85.
[748] M. Qin, Q. Yan, H. Wang, K.S. Vecchio, J. Luo, J. Eur. Ceram. Soc. 41 (2021)
2968–2973.
[749] Y. Zhang, S.K. Sun, W.M. Guo, L. Xu, W. Zhang, H.T. Lin, J. Adv. Ceram. 10
(2020) 173–180.
[750] M. Qin, Q. Yan, Y. Liu, J. Luo, J. Adv. Ceram. 10 (2021) 166–172.
[751] M. Qin, Q. Yan, Y. Liu, H. Wang, C. Wang, T. Lei, K.S. Vecchio, H.L. Xin, T.
J. Rupert, J. Luo, J. Eur. Ceram. Soc. 41 (2021) 5775–5781.
[752] F. Monteverde, F. Saraga, M. Gaboardi, J.R. Plaisier, J. Eur. Ceram. Soc. 41 (2021)
6255–6266.
[753] S. Barbarossa, R. Orrù, V. Cannillo, A. Iacomini, S. Garroni, M. Murgia, G. Cao,
Ceramics 4 (2021) 108–120.
[754] Y. Long, J. Che, Z. Wu, H.T. Lin, F. Zhang, Mater. Chem. Phys. 257 (2021),
123715.
[755] W. Zhang, B. Zhao, N. Ni, H. Xiang, F.Z. Dai, S. Wu, Y. Zhou, J. Mater. Sci.
Technol. 87 (2021) 155–166.
[756] S. Iwan, K.C. Burrage, B.C. Storr, S.A. Catledge, Y.K. Vohra, R. Hrubiak,
N. Velisavljevic, AIP Adv. 11 (2021), 035107.
[757] M. Li, X. Zhao, G. Shao, H. Wang, J. Zhu, W. Liu, B. Fan, H. Xu, H. Lu, Y. Zhou,
R. Zhang, Ceram. Int. 47 (2021) 8707–8710.
[758] B. Storr, D. Kodali, K. Chakrabarty, P.A. Baker, V. Rangari, S.A. Catledge,
Ceramics 4 (2021) 257–264.
S. Akrami et al.
[759] L. Feng, F. Monteverde, W.G. Fahrenholtz, G.E. Hilmas, Scr. Mater. 199 (2021),
113855.
[760] C. Wang, M. Qin, T. Lei, Y. He, K. Kisslinger, T.J. Rupert, J. Luo, H.L. Xin, J. Eur.
Ceram. Soc. 41 (2021) 5380–5387.
[761] S. Barbarossa, R. Orrù, S. Garroni, R. Licheri, G. Cao, Ceram. Int. 47 (2021)
6220–6231.
[762] W. Zhang, B. Zhao, H. Xiang, F.Z. Dai, S. Wu, Y. Zhou, J. Adv. Ceram. 10 (2021)
62–77.
[763] Y. Zhang, S.K. Sun, W.M. Guo, W. Zhang, L. Xu, J.H. Yuan, D.K. Guan, D.
W. Wang, Y. You, H.T. Lin, J. Eur. Ceram. Soc. 41 (2021) 1015–1019.
[764] L. Feng, W.G. Fahrenholtz, G.E. Hilmas, F. Monteverde, J. Eur. Ceram. Soc. 41
(2021) 92–100.
[765] X. Zhang, L. Xu, W. Han, L. Weng, J. Han, S. Du, Solid State Sci. 11 (2009)
156–161.
[766] E. Wuchina, M. Opeka, S. Causey, K. Buesking, J. Spain, A. Cull, J. Routbort,
F. Guitierrez-Mora, J. Mater. Sci. 39 (2004) 5939–5949.
[767] J.W. Zimmermann, G.E. Hilmas, W.G. Fahrenholtz, R.B. Dinwiddie, W.D. Porter,
H. Wang, J. Am. Ceram. Soc. 91 (2008) 1405–1411.
[768] M. Gasch, S. Johnson, J. Marschall, J. Am. Ceram. Soc. 91 (2008) 1423–1432.
[769] J. Francl, W.D. Kingery, J. Am. Ceram. Soc. 37 (1954) 99–107.
[770] M. Hirscher, V.A. Yartys, M. Baricco, J.B. von Colbe, D. Blanchard, R.
C. Bowman Jr., D.P. Broom, C.E. Buckley, F. Chang, P. Chen, Y.W. Cho, J.
C. Crivello, F. Cuevas, W.I.F. David, P.E. de Jongh, R.V. Denys, M. Dornheim,
M. Felderhoff, Y. Filinchuk, G.E. Froudakis, D.M. Grant, E.M. Gray, B.C. Hauback,
T. He, T.D. Humphries, T.R. Jensen, S. Kim, Y. Kojima, M. Latroche, H.W. Li, M.
V. Lototskyy, J.W. Makepeace, K.T. Møller, L. Naheed, P. Ngene, D. Noreus, M.
M. Nygård, S. Orimo, M. Paskevicius, L. Pasquini, D.B. Ravnsbæk, M.V. Sofianos,
T.J. Udovic, T. Vegge, G.S. Walker, C.J. Webb, C. Weidenthaler, C. Zlotea,
J. Alloys. Compd. 827 (2020), 153548.
[771] J. Huot, F. Cuevas, S. Deledda, K. Edalati, Y. Filinchuk, T. Grosdidier, B.
C. Hauback, M. Heere, T.R. Jensen, M. Latroche, S. Sartori, Materials 12 (2019)
2778.
[772] M. Aoki, T. Noritake, A. Ito, M. Ishikiriyama, S. Towata, Int. J. Hydrogen Energy
36 (2011) 12329–12332.
[773] J. Huot, H. Enoki, E. Akiba, J. Alloys. Compd. 453 (2008) 203–209.
[774] R.A. Varin, T. Czujko, Z.S. Wronski, Nanomaterials for Solid State Hydrogen
Storage, first ed., Springer, 2009.
[775] K. Edalati, J. Matsuda, M. Arita, T. Daio, E. Akiba, Z. Horita, Appl. Phys. Lett. 103
(2013), 143902.
[776] K. Edalati, R. Uehiro, Y. Ikeda, H.W. Li, H. Emami, Y. Filinchuk, M. Arita,
X. Sauvage, I. Tanaka, E. Akiba, Z. Horita, Acta Mater. 149 (2018) 88–96.
[777] A. Kazakov, D. Blinov, I. Romanov, D. Dunikov, V. Borzenko, E3S Web Conf. 114
(2019) 05005.
[778] U. Spaliviero, M.G. Poletti, L. Battezzati, M. Baricco, La Metallurgia Itakiana 9
(2019) 14–21.
[779] R.B. Strozi, D.R. Leiva, J. Huot, W.J. Botta, G. Zepon, Int. J. Hydrogen Energy 46
(2021) 25555–25561.
[780] S. Sleiman, J. Huot, J. Alloys. Compd. 861 (2021), 158615.
[781] J. Montero, G. Ek, L. Laversenne, V. Nassif, M. Sahlberg, C. Zlotea, Molecules 26
(2021) 2470.
[782] K.R. Cardoso, V. Roche, A.M.J. Jr, F.J. Antiqueira, G. Zepon, Y. Champion,
J. Alloys. Compd. 858 (2021), 158357.
[783] R. Floriano, G. Zepon, K. Edalati, G.L.B.G. Fontana, A. Mohammadi, Z. Ma, H.
W. Li, R.J. Contieri, Int. J. Hydrog. Energy 46 (2021) 23757–23766.
[784] J. Montero, G. Ek, M. Sahlberg, C. Zlotea, Scr. Mater. 194 (2021), 113699.
[785] J. Liu, J. Xu, S. Sleiman, X. Chen, S. Zhu, H. Cheng, J. Huot, Int. J. Hydrog. Energy
46 (2021) 28709–28718.
[786] K.B. Park, J.Y. Park, Y.D. Kim, J.In Choi, H.T. Im, J.W. Kang, H.S. Kang, T.W. Na,
H.K. Park, Intermetallics 130 (2021), 107074.
[787] G. Ek, Ø.S. Fjellvåg, P. Vajeeston, J. Armstrong, M. Sahlberg, U. Häussermann,
J. Alloys. Compd. 877 (2021), 160320.
[788] R.B. Strozi, D.R. Leiva, J. Huot, W.J. Botta, G. Zepon, Int. J. Hydrogen Energy 46
(2021) 2351–2361.
[789] C. Zhang, A. Song, Y. Yuan, Y. Wu, P. Zhang, Z. Lu, X. Song, Int. J. Hydrogen
Energy 45 (2020) 5367–5374.
[790] J.J. Petrovic, A.K. Vasudevan, Mater. Sci. Eng. A 261 (1999) 1–5.
[791] D.M. Shah, D. Berczik, D.L. Anton, R. Hecht, Mater. Sci. Eng. A 155 (1992) 45–57.
[792] Y.L. Jeng, E.J. Lavernia, J. Mater. Sci. 29 (1994) 2557–2571.
[793] H.C. Kim, C.D. Park, J.W. Jeong, I.J. Shon, Met. Mater. Int. 9 (2003) 173–178.
[794] I.Y. Ko, B.R. Kim, K.S. Nam, B.M. Moon, B.S. Lee, I.J. Shon, Met. Mater. Int. 15
(2009) 399–403.
[795] D.Y. Oh, H.C. Kim, J.K. Yoon, I.Y. Ko, I.J. Shon, Met. Mater. Int. 12 (2006)
307–315.
[796] J.K. Sonber, T.S.R.C. Murthy, K. Sairam, B. Paul, J.K. Chakravartty, Ceram. Int. 42
(2016) 891–896.
[797] H. Wu, in: M. Shokrieh (Ed.), Residual Stresses in Composite Materials, Elsevier,
2014, pp. 256–292.
[798] A.K. Vasudevan, J.J. Petrovic, Mater. Sci. Eng. A 155 (1992) 1–17.
63
Materials Science & Engineering R 146 (2021) 100644
[799] V.S. Neshpor, J. Eng. Phys. 15 (1968) 750–752.
[800] Y. Shen, C. Li, R. Huang, R. Tian, Y. Ye, L. Pan, K. Koumoto, R. Zhang, C. Wan,
Y. Wang, Sci. Rep. 6 (2016) 32501.
[801] H. Zhao, X. Xu, C. Li, R. Tian, R. Zhang, R. Huang, Y. Lyu, D. Li, X. Hu, L. Pan,
Y. Wang, J. Mater. Chem. A 5 (2017) 23267–23275.
[802] K. Chen, B. Du, N. Bonini, C. Weber, H. Yan, M.J. Reece, J. Phys. Chem. C 120
(2016) 27135–27140.
[803] K. Chen, C.D. Paola, B. Du, R. Zhang, S. Laricchia, N. Bonini, C. Weber,
I. Abrahams, H. Yan, M. Reece, J. Mater. Chem. C 6 (2018) 8546–8552.
[804] D. Zhang, J. Yang, Q. Jiang, Z. Zhou, X. Li, J. Xin, A. Basit, Y. Ren, X. He, Nano
Energy 36 (2017) 156–165.
[805] X. Lu, D.T. Morelli, Y. Xia, F. Zhou, V. Ozolins, H. Chi, X. Zhou, C. Uher, Adv.
Energy Mater. 3 (2013) 342–348.
[806] K. Suekuni, K. Tsuruta, T. Ariga, M. Koyano, Appl. Phys. Express 5 (2012),
051201.
[807] A. Lucca, M. Jacquemet, F. Druon, F. Balembois, P. Georges, P. Camy, J.
L. Doualan, R. Moncorgé, Opt. Lett. 29 (2004) 1879–1881.
[808] M. Siebold, M. Hornung, R. Boedefeld, S. Podleska, S. Klingebiel, C. Wandt,
F. Krausz, S. Karsch, R. Uecker, A. Jochmann, J. Hein, M.C. Kaluza, Opt. Lett. 33
(2008) 2770–2772.
[809] H. Saito, Y. Nagashima, T. Kurihara, T. Hyodo, Nucl. Instrum. Methods Phys. Res.
A 487 (2002) 612–617.
[810] M.A. Nelson, B.D. Rooney, D.R. Dinwiddie, G.S. Brunson, Nucl. Instrum. Methods
Phys. Res. A 505 (2003) 324–327.
[811] A.A. Demidenko, E.A. Garibin, S.D. Gain, Y.I. Gusev, P.P. Fedorov, I.A. Mironov,
S.B. Michrin, V.V. Osiko, P.A. Rodnyi, D.M. Seliverstov, A.N. Smirnov, Opt.
Mater. (Amst) 32 (2010) 1291–1293.
[812] A.J. Stevenson, H. Serier-Brault, P. Gredin, M. Mortier, J. Fluor. Chem. 132
(2011) 1165–1173.
[813] A. Lyberis, A.J. Stevenson, A. Suganuma, S. Ricaud, F. Druon, F. Herbst, D. Vivien,
P. Gredin, M. Mortier, Opt. Mater. (Amst) 34 (2012) 965–968.
[814] Z. Liu, B. Mei, J. Song, W. Li, J. Eur. Ceram. Soc. 34 (2014) 4389–4394.
[815] Z. Liu, B. Mei, J. Song, D. Yuan, Z. Wang, J. Alloys. Compd. 646 (2015) 760–765.
[816] W. Li, Z. Liu, Z. Zhou, J. Song, B. Mei, L. Su, J. Eur. Ceram. Soc. 36 (2016)
3481–3486.
[817] F. Nakamura, T. Kato, G. Okada, N. Kawaguchi, K. Fukuda, T. Yanagida, J. Eur.
Ceram. Soc. 37 (2017) 4919–4924.
[818] Z. Sun, B. Mei, W. Li, X. Liu, L. Su, Opt. Mater. (Amst) 71 (2017) 35–40.
[819] Z. Liu, M. Jia, G. Yi, B. Mei, Q. Jing, P. Liu, J. Am. Ceram. Soc. 102 (2019)
285–293.
[820] T. Kato, G. Okada, K. Fukuda, T. Yanagida, Radiat. Meas. 106 (2017) 140–145.
[821] P.P. Fedorov, S.V. Kuznetsov, A.N. Smirnov, E.A. Garibin, P.E. Gusev, M.
A. Krutov, K.A. Chernenko, V.M. Khanin, Inorg. Mater. Appl. Res. 50 (2014)
738–744.
[822] J. Li, X. Chen, L. Tang, Y. Li, Y. Wu, J. Am. Ceram. Soc. 102 (2019) 178–184.
[823] W. Li, B. Mei, J. Song, Z. Wang, Mater. Lett. 159 (2015) 210–212.
[824] W. Li, H. Huang, B. Mei, J. Song, Opt. Mater. (Amst) 75 (2018) 7–12.
[825] P.A. Sukkurji, Y. Cui, S. Lee, K. Wang, R. Azmi, A. Sarkar, S. Indris, S.
S. Bhattacharya, R. Kruk, H. Hahn, Q. Wang, M. Botros, B. Breitung, J. Mater.
Chem. A 9 (2021) 8998.
[826] Y. Pei, Y. Cheng, J. Chen, W. Smith, P. Dong, P.M. Ajayan, M. Ye, J. Shen,
J. Mater. Chem. A 6 (2018) 23220–23243.
[827] K. Liu, C. Zhang, Y. Sun, G. Zhang, X. Shen, F. Zou, H. Zhang, Z. Wu, E.
C. Wegener, C.J. Taubert, J.T. Miller, Z. Peng, Y. Zhu, ACS Nano 12 (2018)
158–167.
[828] J. Xu, J. Li, D. Xiong, B. Zhang, Y. Liu, K.H. Wu, I. Amorim, W. Li, L. Liu, Chem.
Sci. 9 (2018) 3470–3476.
[829] H. Qiao, X. Wang, Q. Dong, H. Zheng, G. Chen, M. Hong, C.P. Yang, M. Wu, K. He,
L. Hu, Nano Energy 86 (2021), 106029.
[830] S. Bolognini, G. Feusier, D. Mari, T. Viatte, W. Benoit, Int. J. Refract. Metals Hard
Mater. 16 (1998) 257–268.
[831] H. Zhang, S. Tang, J. Yan, X. Hu, Int. J. Refract. Metals Hard Mater. 25 (2007)
440–444.
[832] S. Ma, J. Ma, Z. Yang, Y. Gong, K. Li, G. Yu, Z. Xue, Int. J. Refract. Met. Hard
Mater. 94 (2021), 105390.
[833] Z. Peng, W. Sun, X. Xiong, H. Zhang, F. Guo, J. Li, Corros. Sci. 184 (2021),
109359.
[834] P. Zhang, X. Liu, A. Cai, Q. Du, X. Yuan, H. Wang, Y. Wu, S. Jiang, Z. Lu, Sci.
China Mater. 64 (2021) 2037–2044.
[835] T. Wen, B. Ye, M.C. Nguyen, M. Ma, Y. Chu, J. Am. Ceram. Soc. 103 (2020)
6475–6489.
[836] S.C. Luo, W.M. Guo, K. Plucknett, H.T. Lin, J. Eur. Ceram. Soc. 41 (2021)
3189–3195.
[837] M. Qin, J. Gild, C. Hu, H. Wang, M.S.B. Hoque, J.L. Braun, T.J. Harrington, P.
E. Hopkins, K.S. Vecchio, J. Luo, J. Eur. Ceram. Soc. 40 (2020) 5037–5050.
S. Akrami et al. Materials Science & Engineering R 146 (2021) 100644

Saeid Akrami obtained a MSs degree in Chemical Engineering Masayoshi Fuji is currently a professor of Advanced Ceramics
and he is currently a PhD candidate in Applied Chemistry and Research Center, Nagoya Institute of Technology, Tajimi,
Life Sciences in Nagoya Institute of Technology, Japan. The Japan and a visiting professor and joint researcher in Beijing
topic of his PhD study is the development of highly-strained University of Chemical Technology, the Chinese Academy of
and high-entropy ceramics for CO2 conversion. Sciences and Osaka University. He received his BSc, MSc and
PhD degrees in the field of industrial chemistry from Tokyo
Metropolitan University. He worked in Tokyo Metropolitan
University and the University of Florida before joining Nagoya
Institute of Technology in 2002. He is the editor-in-chief of the
journal of Advanced Powder Technology. His research interests
are surface/bulk chemistry of various kinds of multifunctional
ceramics and their processing. Among his research activities,
the development of hollow particle ceramics and the introduction of non-firing solidifi­
cation technique for oxides have received high scientific and industrial attention and led to
several awards including an award from the minister of education, culture, sports, science
and technology of Japan in 2013.
Parisa Edalati is a PhD candidate in the Advanced Ceramics
Research Center, Nagoya Institute of Technology, Japan. She
currently works on the design and synthesis of advanced high-
entropy ceramics for water splitting and battery applications. Kaveh Edalati obtained a PhD degree in materials physics and
As a visiting researcher in Kyushu University, she worked and chemistry from Kyushu University, Fukuoka, Japan, in 2010.
published a few papers on high-entropy alloys for biomedical He is currently an associate professor at the International
application, high-entropy hydrides for hydrogen storage and Institute for Carbon-Neutral Energy Research, Kyushu Univer­
high-entropy oxides/oxynitrides for photocatalysis. sity, Fukuoka, Japan. His current research interest is the
development of functional energy materials for hydrogen-
related applications such as hydrogen storage and photo­
catalytic hydrogen generation. He specifically employs severe
plastic deformation through the high-pressure torsion process
to develop new functional materials including high-entropyy
alloys and ceramics. He is the author of over 150 journal pa­
pers and serves as the editor of several journals.

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