Ti3C2Tx Mxene: From Dispersions To Multifunctional Architectures For Diverse Applications

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Ti3C2Tx MXene: From Dispersions to Multifunctional Architectures for

Diverse Applications
Article in Materials Horizons · August 2021

DOI: 10.1039/D1MH00968K
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DOI: 10.1039/D1MH00968K
REVIEW
Ti3C2Tx MXene: From Dispersions to Multifunctional Architectures

for Diverse Applications
Materials Horizons Accepted Manuscript

Received 00th January 20xx, Ken Aldren S. Usman,a Si Qin,a Luke C. Henderson,a Jizhen Zhang,a Dylan Y. Hegh,a* Joselito M.
Accepted 00th January 20xx Razala*
Published on 17 August 2021. Downloaded by Deakin University on 8/17/2021 1:31:55 AM.
DOI: 10.1039/x0xx00000x The exciting combination of high electrical conductivity, high specific capacitance and colloidal stability of two-dimensional
Ti3C2Tx MXene (referred to as MXene) has shown great potential in a wide range of applications including wearable
electronics, energy storage, sensors, and electromagnetic interference shielding. To realize its full potential, recent literature
has reported a variety of solution-based processing methodologies to develop MXenes into multifunctional architectures,
such as fibres, films and aerogels. In response to these recent critical advances, this review provides a comprehensive
analysis of the diverse solution-based processing methodologies currently being used for MXene-architecture fabrication. A
critical evaluation of the processing challenges directly affecting macroscale material properties and ultimately, the
performance of the resulting prototype devices is also provided. Opportunities arising from the observed and foreseen
challenges regarding their use are discussed to provide avenues for new designs and realise practical use in high performance
applications.
MXenes, Ti3C2Tx has been the most studied, possessing

Introduction unprecedented electrical conductivity (~20,000 S cm-1)20, 21 and
volumetric capacitance (~1,500 F cm-3)22 compared with other
In response to the rapidly growing technology, numerous
2D materials. Additionally, this Ti based MXene is also
multifunctional materials with remarkable properties are either
hydrophilic, resulting in good aqueous colloidal stability (zeta-
continuously discovered and/or developed into functional
potential -30 to -60 mV) with versatile solution processability,
architectures. As an example, materials with inherently high
even in the absence of additional binders or surfactants.23, 24
conductivity and mechanical strength such as carbon
Moreover, a growing understanding of its rheological
nanotubes,1-3 graphene,4-7 and carbon fibres8 are being
behavior25, 26 and dispersibility in a variety of polar organic
constantly tailored to introduce interesting functions such as
solvents27-29 has enabled the development of multiple
energy conversion/storage9-11 and/or electromagnetic
processing methods allowing the production of new
interference (EMI) shielding,12 enabling their use in practical
architectures and geometries such as fibres,26 and porous 3D-
applications. Examples of these applications include more
structures.30
efficient and safer batteries and/or supercapacitors for vehicles
These recent discoveries have propelled MXene towards
and electronics,13, 14 and more accurate and sensitive
practical use in applications including; energy storage,31, 32
components in healthcare monitoring devices.10, 15 Recently, a
energy harvesting,33, 34 sensors,35, 36 actuators,37, 38
new series of two-dimensional transition metal carbides and/or
electromagnetic interference shielding,39, 40 and
nitrides called MXenes (Mn+1XnTx, n = 1 to 4, where M =
photo/electrocatalysis. 41, 42 Moreover, several studies have
transition metal, X = carbon and/or nitrogen, and Tx = –F, –O,
been dedicated towards innovating conventional MXene-based
and/or –OH) have gained significant attention due to their
functional architectures such as films,30, 43 fibres9, 44-47 and
outstanding properties, particularly their unique combination
foams25, 48 for use in targeted applications. With these rapid
of excellent electrical and electrochemical properties.16-18 Since
developments, excellent reviews have been published on the
their discovery in 2011,16 over 30 MXene varieties have been
preparation and application of MXene and MXene-composites
synthesized, with dozens more unique structures and
(e.g., batteries, membranes, etc.).9, 44-47, 49-51 There are also
properties theoretically predicted.19 Among all synthesized
several articles that have highlighted the importance of
rheological behavior and/or dispersibility of MXene in various
a. Institutefor Frontier Materials, Deakin University, Geelong, VIC, 3216, Australia. solvents towards the development of materials in these
Email: Dr. D. Y. Hegh (dylan.hegh@research.deakin.edu.au),. Prof. J. M. Razal applications.25, 48 Nevertheless, recent critical advances in
(joselito.razal@deakin.edu.au).
† Footnotes relating to the title and/or authors should appear here.
solution-based processing of MXenes calls for the need to
Electronic Supplementary Information (ESI) available: [details of any supplementary systematically discuss how MXene dispersions can be tuned
information available should be included here]. See DOI: 10.1039/x0xx00000x
Please do not adjust margins

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DOI: 10.1039/D1MH00968K

Fig.1. Illustration depicting the major steps in developing MXene-based architectures. The device design begins with acquiring MXene flakes with optimal properties thorough
choice of suitable etching method, followed by careful dispersion in the appropriate solvent to inhibit oxidation or destruction into smaller flakes. Since different processes used
to fabricate macroscale architectures of MXene (i.e., thin-film coating, fibre spinning, etc.) are highly dependent on the rheological properties of its dispersion (e.g., viscosity, and
elastic and viscous moduli), understanding of such fundamental properties allows us to carefully select a suitable strategy on which a certain MXene dispersion can be fabricated
in an optimal architecture for subsequent inclusion in a device for a targeted practical application.
(e.g., flake size, solvent concentration, and rheological “MAX” phase (Figure 2a). These MAX phases comprise of
properties, etc.) for fabricating different functional alternating transition metal carbides or nitride (MX) layers and
architectures. Hence, in this review, we provide a “A” atoms composed of group 13 or 14 elements.16
comprehensive discussion of solution based MXene processing Furthermore, variations in etchant solution conditions result in
methodologies, and critically evaluate the processing different yield, quality, layered structure, and surface
challenges that influence macroscale material properties and, termination of MXene. The following section briefly reviews the
ultimately, the performance of the resultant device (Figure 1). development of MXene synthesis and the factors influencing its
In particular, this article focuses on characteristics of MXene structural properties, deemed crucial for the development of
dispersions (surface chemistry, flake size, solvent MXene-based macroscale architectures.
concentration, and rheological properties, etc.) required for a
specific method in fabricating a desired functional architecture. Synthesis of MXenes
We also describe how flake alignment, directional pores and Generally, the MAX phase A layer, typically being aluminium
tailored interfaces in MXene architectures are used to modulate (Al), is selectively removed with F- using an aqueous solution of
strength, electrical conductivity and ion transport. Finally, we hydrofluoric acid (HF)-containing or HF-forming etchant.9, 52
discuss the processing challenges of MXene dispersions and Based on DFT calculations, a large negative formation energy
offer insights on potential strategies to circumvent their exists when the transition metal of the Mn+1Xn layers is exposed
vulnerability towards oxidation. to functionalities such as -O, -OH, and/or -F.16, 53, 54 This indicates
strong bond formation potential between the transition metal
and the -O, -OH, and/or -F groups of the aqueous etchant (e.g.,
Synthesis and properties of MXene
HF, ammonium bifluoride (NH4HF2) or LiF/HCl) solution
MXenes are commonly produced by selectively etching the compensating for the structural vacancies generated through
atomic layer “A” from parent layered structures, called the loss in coordination upon removal of the “A” layer.16, 54
2 | J. Name., 2012, 00, 1-3 This journal is © The Royal Society of Chemistry 20xx

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Materials Horizons REVIEW
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DOI: 10.1039/D1MH00968K

Fig.2. MXene synthesis producing multi-layer and/or single-layer MXenes. a) Schematic illustrating the process of removing Al from Ti3AlC2 to produce Ti3C2Tx MXene. Termination
groups (such as -OH and –F) are shown on the surface of MXene flakes, along with interlayer water. b) SEM images showing the morphological evolution of MAX phase into multi-
layer MXene and delaminated single-layer flakes. Adapted with permission.11 Copyright © 2017 The Royal Society of Chemistry.
Furthermore, the ratio of -O, -OH, and/or -F terminations on the dimethysulfoxide (DMSO),57 dimethyl formamide (DMF)57) or
MXene surface can be modified by varying either the etchant or organic base (e.g., tetramethyl ammonium hydroxide
etching parameters.23, 24 Aside from providing structural (TMAOH)58) to swell the MXene layers followed by sonication-
stability to the transition metal-carbide/nitride backbone, these assisted delamination, is usually required. However, sonication-
terminations directly influence the electrical/electrochemical assisted delamination decreases lateral flake size from
behaviour and other properties such as sorption and catalytic micrometers to a few hundred nanometers, leading to
capabilities.19, 55, 56 mechanical and electrical properties.59 In order to control flake-
Early etching methods involved the exposure of MAX to size, surface termination and yield, new synthetic approaches
different concentrations of HF solutions at varying have been developed, such as the mixed-acid46, 60, 61 and
temperatures.52 However, the strong interlayer interactions minimally intensive layer delamination (MILD) methods59, 62. It
between MXene flakes, up to six-fold stronger than those of should be noted that although desirable, unfortunately to date,
other 2D materials (e.g., graphite and MoS2),9 resulted in the few studies on MXene synthesis report yield rendering a
formation of multi-layer structures (Figure 2b). Therefore, to comparison of the efficiency of the various methodologies
exfoliate the more desirable fully solvated single-layered flakes, difficult.
an intercalation step using either an organic solvent (e.g.,
Ken Aldren S. Usman is a PhD Dylan Y. Hegh is currently a

candidate at the Institute for Research Engineer for the
Frontier Materials, Deakin Australian National
University under the Fabrication Facility (ANFF)
supervision of Prof. Joselito M. Victorian Node at Deakin
Razal. His research interests University. His recent works
include synthesis and surface focuses on the development of
modification of nanomaterials, functional fibres, with an
and processing of functional emphasis on materials
architectures. His current work chemistry and sustainable
focuses on developing manufacturing. He is also
structurally fortified Ti3C2Tx- actively working alongside a
MXene-based materials with number of industry partners,
uncompromized electrical and electrochemical performance. He for projects involving translating bench-scale advanced fibre
received his BS and MS degrees from the University of the research into commercial prototypes. He received his PhD from
Philippines in 2013 and 2018, respectively. the University of Otago in 2014.
This journal is © The Royal Society of Chemistry 20xx J. Name., 2013, 00, 1-3 | 3

PleaseMaterials
The mixed-acid method uses an HCl/HF/H2O etching Ti3C2Br2 is heated with Li2Se,26 consequently enabling control
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solution (6:1:3) which results in a more complete etching of over the surface chemistry, structure, and properties
DOI: of MXene
10.1039/D1MH00968K
MAX into multi-layer MXene, followed by a secondseparate materials. Halogen etching (using ~10% v/v Br2, I2 and/or Cl2 in
delamination step vortexed with an intercalating agent, such as cyclohexane) of MAX at RT (8 h) has been also explored
LiCl.61, 63 In contrast, the MILD method involves mixing of lithium producing Br, I, and/or Cl-terminated multi-layer MXenes,
fluoride (LiF) powder into a solution of hydrochloric acid (HCl), which were then delaminated into single-layer flakes using
where the dissociated F- etches and Li+ ions subsequently either tetrabutylammonium bromide (TBAB) or HCl(aq).70 Finally,
delaminates, in a one-pot synthesis.26, 59, 64 Although the former a safe, efficient (in milliseconds) acid-free method to etch
method also produces sonication free fully-delaminated single single-layer MXene has been demonstrated using aqueous LiF
layer MXene flakes, the one-step MILD method (self- (as Li+ and F- source) induced by surface acoustic waves
delamination enabled by Li-ion intercalation and abundant –OH (SAWs).71 In this approach, the very high surface acceleration

terminations), is generally preferred since it also yields large imparted my SAWs (∼108 m s–2) provides sufficient energy to
flake size (> 2 μm) and minimises the formation of defects.9 weaken the MAX Ti-Al bonds and quickly dissociates the Li+ and
Further modifications of the MILD method includes tuning flake F- ions (at significantly faster rates than regular stirring) even at
size using elevated temperatures (~40 ℃ vs. Room Temperature a low LiF concentrations (0.05 M vs. ~3 M for the MILD method).
(RT)) to produce extremely large flakes (> 10 µm).59 However, However, high energy etching methods such as this is known to
the recurring safety issues involving the use and generation of reduce flake size.9, 59, 71
HF limits the scalability of all these methods, from handling of Despite providing feasible alternative to HF-based etching,
raw materials to the disposal of highly corrosive solvent waste. the current drawbacks of these non-HF generating methods
To mitigate such hazards, NH4HF2 dissolved in an organic polar include incomplete Al removal and small flake size, which affect
aprotic solvent (e.g., propylene carbonate),65 has been explored physical,59 electrical,9, 59 and electrochemical properties72. As
as a relatively safer alternative fluoride-based etchant. alternative etchants (halogens, TMAOH, etc.) are larger
Dissociation into NH4F and HF allows the removal of Al layers compared to F- they are unable to intercalate into the MAX Al
with significantly lower production of HF, while also reducing layer as effectively. Meanwhile the molten salt method, being a
the handling risk of aqueous HCl and HF (e.g., less dissociation solid-state solvent-free approach faces difficulties in complete
of HCl into H+ and Cl-).65 removal of trapped Al impurities from the multilayer flakes.
Production techniques that completely avoid the use or Therefore, despite recent advances in alternative etching
generation of extremely hazardous HF have been also explored. processes, a HF wet etching approach is preferred for MXene
Base etching approaches include treating MAX with organic synthesis due to its superior product, quality and production
base TMAOH, followed by exposure of the reaction media to cost.
electrical currents.66 More exotic methods include the
production of thermodynamically unstable MAX from Ti3AlC2 by Properties of MXenes
in-situ replacement of Al with Zn, Cu or Cd by sintering in Ar Mechanical properties. The mechanical properties from
atmosphere at elevated temperature (~550 ℃ - ~750 ℃) with nanoindentation experiments of MXene flakes show a Young’s
molten ZnCl2,67-69 CuCl2,67-69 and CdBr269 salts, respectively, modulus of ~330 GPa for MXene, higher than either GO (~210
followed by simple aqueous delamination. These Cl- and Br- GPa) or rGO (~250 GPa).73 According to DFT calculations, this
terminated MXenes are capable of engaging in a new type of exceptional strength is due to extensive surface
surface reaction such as halide ion exchange for specific atoms functionalization, which inhibits tensile/strain induced collapse
and functional groups, for example forming Ti3C2Se when at the atomic level of the MXene flake.74 It is predicted that
formation of -O- terminal functionalities after etching results in
a larger elastic constant (Young’s modulus) compared to -F, -OH,
Joselito M. Razal is a Professor
or unterminated MXene. This behavior is ascribed to the
at the Institute for Frontier
stronger coordination between -O and surface transition
Materials, the Deputy Director
metals, inhibiting surface defects.72, 75, 76 On the other hand, a
of the Australian Research
simulated un-functionalized MXene flake is predicted to
Council Research Hub for
undergo a c-lattice parameter contraction of 19%,16 as exposed,
Future Fibers at Deakin
uncoordinated, Ti on the MXene surface is relatively unstable
University, and ARC Future
which induces steric stress on the nanostructure, making it
Fellow. His research interest is
more prone to structural collapse.16
focused around functional
Electrical properties. Another striking property of MXenes
ﬁbers that can be integrated
is their metal-like electrical conductivity, up to ~11,000 S cm-177
into wearable devices, portable
for monolayer flakes and ~20,000 to 24,000 S cm-120, 21 for films
electronics, bioelectronic
of Ti3C2Tx. DFT calculations have shown that MXenes have
interfaces, and smart textiles.
remarkably high density of states (DOS) at the Fermi level75 and
As well as the development of wearable energy storage and
this conductivity can be tuned through its surface terminations,
energy harvesting systems using high aspect ratio MXenes and
as these electrons withdrawing groups (-O, -OH, -F) share
graphene oxide.

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electrons from the arranged MX backbone.78 Furthermore, block the ion-transfer towards redox active sites.View
85 Therefore,
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these surface terminations can cause a significant downward intercalants, such as polar organic molecules and cations (e.g.,
DOI: 10.1039/D1MH00968K
shift on the MXene’s Fermi energy level, lowering conductivity, hydrazine86 and ammonium84, 87, 88), have been widely used to
resulting in a band gap, and inducing semi-conductivity.79 increase MXene inter-flake spacing to efficiently ease
Although semi-conductivity of Ti3C2Tx has not been electrolyte access resulting in better device performance.
experimentally observed, semi-conductivity of fully surface-
terminated bi-metallic MXenes (Mo2TiC2Tx and Mo2Ti2C3Tx), has MXene dispersions
been reported.53, 80-82 Delamination of multilayer-MXene into stable dispersions of
Electrochemical properties. MXenes are also uniquely single/few-layer flakes is an important first step toward the
suited for energy storage applications, with reported volumetric processing of multi-functional architectures. As discussed
capacitance up to 1500 F cm-3 (Ti3C2Tx).22, 83, 84 MXenes are

previously, a variety of delamination techniques has been
known to exhibit both electrical double layer capacitance reported such as cation,84, 89, 90 surfactant,91 and/or
(EDLC), through the ability to form electrical double layer at the solvent/guest molecule intercalation (e.g., DMSO/DMF,57
interface of its negatively charged surface, and pseudo- hydrazine86) followed by ultrasonication. However, the demand
capacitance, enabled by its transition-metal carbide/nitride for simple and scalable production of high quality single-layer
redox sites. This dual behaviour can be tuned through surface flakes has led to the optimized one-step MILD method. The
groups, as their electron withdrawing nature improves the MXene flakes acquired through this approach exhibit excellent
negative surface charge increasing cation affinity. As an dispersibility in water due to increased functional group surface
example, favourable sites (e.g., electron rich –O and –OH coverage.27 Initial studies in tuning the rheological behavior of
groups) for Li+ ion insertion into functionalized MXene improves MXene have also demonstrated that flake size, concentration
the operation voltage and capacity of the system55. However, and solvent choice are also critical factors for several solution
presence of terminations and additional surface groups (either processing techniques including spin coating,92 spray coating,93
adsorbed from etchant or presence of oxidation sites) may also drop-casting,94 and ink-jet printing.95 The subsequent section
Fig.3. Rheological and LC properties of MXene dispersions. a) Frequency dependence of the ratio of G′ (the elastic modulus) to G″ (the viscous modulus) for single-layer MXene
flakes dispersed in water. Adapted with permission.25 Copyright © 2018 American Chemical Society, b) Theoretical calculations of the relationship between the lateral size of
MXene flakes and the concentration for the isotropic to LC phase transformation (CT). The red star and black star represent the experimental results for large size and small size
MXene flakes, respectively. Adapted with permission.26 Copyright © 2020 American Chemical Society

PleaseMaterials
summarises the key parameters to be considered in the bromide (CTAB) stabilized-carbon nanotube (CNT)-MXene LC
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preparation of solution-stable MXene dispersions with high enabled the formation of films with vertically aligned flakes.92
DOI: 10.1039/D1MH00968K
concentration for optimum processability.. Vertical orientation allowed thickness-independent ion
Rheological properties. Understanding the rheological transport, resulting in improved rate performance relative to
properties of 2D materials in dispersed state is critical for the neat MXene films.92 More recently, the formation of pure
development of various solution processing and manufacturing Ti3C2Tx MXene LC dispersions made it possible to produce pure
techniques. Recent studies on MXene dispersions have shown fibers for the first time using a wet-spinning method.26, 104, 105
that film and fibre fabrication is highly dependent on the These fibers exhibit high conductivity (~7,750 to 12,500 S cm-1)
rheological properties (e.g., viscosity, elastic moduli (G’), that surpasses all existing 2D-nanomaterial-based fibers (e.g.,
viscous moduli (G’’) and G’/G’’ ratio).25, 26, 48 For example, a ~380 S cm-1 for graphene fibers).106
highly viscous MXene dispersion that demonstrates shear- Influence of flake size. Flake size, defined as the longest

thinning behavior is generally suitable for fibre wet-spinning, dimension (w) of the particle (Figure 4a), plays an important
provided a high G’/G” ratio (>1) which ensures that the resulting role on the rheological behavior of MXene dispersions. From
architecture is retained after shear force removal. (Figure 3a).96 recent reports flake sizes up to 10 µm have been obtained,59
These parameters can be tuned through either adjusting the however for the following discussions, we will consider flakes
volume fraction (via flake size-selection) or the concentration of >2 µm as the benchmark for large size. Recent studies
MXene dispersions.48, 96, 97 As summarized in Figure 3a, this demonstrate that dispersions of large MXene (~3 μm) exhibits a
concept applies for most processing methods including but not high yield stress viscosity of ~5,000 Pa•s at a substantially lower
limited to wet-spinning, spray coating and dry-spinning. concentration (~27 mg mL-1), compared to small flakes (~310
MXene liquid crystals. Aside from rheological behavior, the nm, ~150 mg mL-1).26 Large MXene also exhibits a strong
discovery of liquid crystal (LC) ordering in two-dimensional (2D) dominance of G’ over G” throughout the frequency range of 10-
materials, including MXenes, have enabled new processing 2 to 102 Hz. These results indicate that large flakes already
methodologies for the production of 3D macrostructures with exhibit viscoelastic gel-like properties even at low
unique properties.98-100 LCs are thermodynamically stable concentrations, easily achieving the required criteria for most
mesophases that simultaneously exhibit liquid-like fluidity and processing methods compared with small flakes. It was also
crystal-like order.101-103 The hydrophilic transition metal oxide reported that the critical transition concentration (Ct) to exhibit
and hydroxide bonds on the MXene basal plane allows LC behaviour has an inverse dependence on flake size (Figure
nanoflake ordering and alignment, which can be tuned mostly 3b), meaning that a dispersion of ~2 μm flakes should exhibit LC
by changing the concentration,26, 59, 101 temperature,101 and behaviour at concentration higher than ~10 mg mL-1.26, 59 In fact,
application of shear26, 59, 101 (Figure 3b). As an example, LC dispersions of very large flakes (8 μm) exhibited an elastic
mechanical shearing of a mixed cetyltrimethylammonium
Fig.4. Refining MXenes towards the desired flake size. a) Schematic illustration of the chemical structure of MXene flakes showing how its dimensions are typically reported.
Adapted with permission.26 Copyright © 2020 American Chemical Society. b) SEM and AFM images of small and large MXene flakes. Adapted with permission.108 Copyright ©
2020 Wiley-VCH. c) Modified synthetic process to produce large MXene flakes from pre-selected large MAX particles. Adapted with permission.59 Copyright © 2020 Wiley-VCH

Horizons
modulus of ~36,500 Pa at a concentration of 50 mg mL−1, Preventing MXene oxidation in dispersion. The presence
View of
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sufficient for 3D printing (Figure 3a).25 surface terminations (Figure 2a) causes MXene
DOI: to exhibit a
10.1039/D1MH00968K
However, typical MXene dispersions often exhibit relatively low zeta potential in the range of -30 to -60 mV (at pH
undesirable lateral-size polydispersity. Thus, several strategies 7),109, 110 allowing easy water dispersion. However, one
to control both the flakes size and distribution have been notorious limitation of fabricating MXenes into suitable
reported,107 as discussed previously, the synthetic method structures and devices is that, like other 2D-nanomaterials (e.g.,
significantly affects the flake-size distribution such that those phosphorenes),[4] they are susceptible to oxidation when stored
requiring additional sonication-assisted delamination (e.g., HF- in water at room temperature, only lasting for up to a couple of
method) result in dispersions with narrow size distributions, but days.111 This oxidation leads to degradation of their structural
with small flake sizes (~100 nm to 300 nm) (Figure 4b).62, 108 On morphology from flakes into particles (mixed Ti3C2Tx and TiO2),
the other hand, self-delaminated MXene synthesized by the and lowering properties such as electrical conductivity and

MILD or mixed-acid method leads to larger flakes with a large capacitance. Investigations into the preservation of MXene has
size distribution (~100 nm to 10 μm), implying sonication demonstrated that oxidation was driven by the presence of
destroys large MXene flakes (Figure 4b). To narrow the dissolved oxygen in the dispersing media (water).27, 28 Efforts to
distribution, large (>2 μm) and small (<300 nm) flakes are overcome this challenge showed that oxidation rates can be
subsequently separated using their mass difference through slowed down by degassing the water prior to dispersing MXene
either a sucrose density gradient107 or differential sediment.62 It was also found out that addition of significant
centrifugation.62, 108 Although these techniques allow selective amounts of anti-oxidants such as sodium L-ascorbate (100 mg
separation selection of large and small MXene flakes, pre- vs 0.6 mg MXene) enables MXene to resist oxidation for up to
etched size selection of large MAX particles gives uniformly 21 days (Figure 5a).112
distributed large MXene flakes (>10 μm) without additional However, another challenge with aqueous MXene
processing (Figure 4c). 59 dispersions is that a wide range of polymers and other materials
Fig.5. Methods to circumvent MXene oxidation. a) Addition of anti-oxidants such as sodium L-ascorbic acid enables MXene flakes to resist oxidation for up to 21 days. Adapted
with permission.12 Copyright © 2019 Elsevier Inc. b) Schematic illustration of the solvent exchange processing approach and the digital photographs and SEM images of the
dispersions in vials 28 days after processing. Adapted with permission.36 Copyright © 2019 Wiley-VCH. c) Temperature dependence of MXene oxidation showing that freezing
aqueous MXene dispersions down to a range of -20 to -80℃ to prolong its shelf-life up to nearly 2 years. TEM images showing no distinct difference in morphology for freshly
synthesized and MXene frozen for 650 days. Adapted with permission.48 Copyright © 2020 American Chemical Society

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are incompatible with water, limiting the number of possible successfully prolong its shelf-life from tens of daysView
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composite architectures that can be constructed. To address 2 years, maintaining flake morphology, chemical properties and
DOI: 10.1039/D1MH00968K
this issue, dispersing MXene in organic solvents, through a electrical conductivity.113, 116
simple solvent exchange (SE) processes consisting of repeated
centrifugation and manual shaking has been investigated
(Figure 5b).27, 28 Compared to other known processing Solution processing of MXene dispersions
approaches, such as re-dispersion of dried MXene powder into Insights on the fundamental properties of MXenes (e.g.,
organic solvents, which often results to non-homogeneous conductivity, capacitance) and their properties in dispersion,
dispersions incapable of being processed into composites,27, 29 particularly the detailed study of rheological behavior and
SE is additive-free, sonication-free, and highly versatile as discovery of their LC phases, has led to the development of
multiple solvent transfers can be carried out in sequence to

processing techniques enabling novel macrostructures with
yield MXene dispersions in a broad variety of solvents. This unique properties. As an example, it was shown for the first
approach is also a potential storage methodology with time that LC-MXene dispersions can be prepared without LC
dispersions stable at room temperature for up to 30 days (using inducing additives, binders, or stabilizing agents, which can be
a variety of solvents such as DMSO, DMF and NMP), with processed into novel architectures (e.g., films of vertically
retention of solution processability demonstrated by the aligned flakes).26 The following section provides a summary of
formation of conductive composite fibres from the stored the current design principles and requirements of various
dispersion.28 Recently, a method involving dispersing MXenes in fabrication methods and recent advances in the production of
the deep eutectic solvent choline chloride and urea in ethylene pure and composite architectures from MXene dispersions. The
glycol was found to prolong the oxidation process up to ~28 various processing methods are analyzed to ascertain which key
weeks due to the high concentration of H-bond accepting and MXene dispersion properties (e.g., flake size, concentration,
donating molecules on the MXene surface hindering contact dispersant) are critical to achieve the manufacture of MXene
with dissolved oxygen.114 This method was also found to architectures and devices. It is important to note that these
functionalize the surface of MXene with urea, enabling methods all utilize MXene dispersions, wheresas processes such
protection against oxidation even when dried. as atomic layer and chemical vapour deposition fall outside the
A drawback of the aforementioned MXene storage scope of this review.
methods is that retention of solvent or additives in MXene
architectures after processing leads to a decrease in electrical Free-standing films
conductivity.11, 28, 115 To overcome these hurdles, additive-free
The limited dispersibility of early MXenes consisting of multi-
long-term aqueous MXene storage has recently been
layered flakes also made them extremely prone to
demonstrated using a low-temperature preservation (freezing)
agglomeration, hence, early methods of fabricating MXene-
method (Figure 5c).113, 116 Such techniques are a common
based films involved flattening ‘clays’ with the aid of rollers.83
strategy to prevent degradation of biological materials and is
The rapid growth in understanding the delamination process of
widely used in food preservation,117 biochemical research118
MXenes enabled subsequent expansion of film-processing
and medical surgery.119 It was found that decreasing the storage
methodologies. As of now, MXene dispersions are usually
temperature of aqueous MXene dispersions to below -20 ℃ can
Fig.6. Approaches used to fabricate free-standing MXene-films. a) Flux-induced stacking of MXene flakes through VAF. Adapted with permission.23 Copyright © 2021 Wiley-VCH.
b) Shear-induced flake alignment in LC-MXene dispersion using BC producing continuous, strong, and dense films. Adapted with permission.39 Copyright © 2020 Wiley-VCH

Horizons
fabricated into films using vacuum assisted filtration (VAF), Substrate-supported films View Article Online
were ordered layering of 2D nanoflakes is induced by DOI: 10.1039/D1MH00968K
Depositing a thin layer of MXene on substrates, such as glass,
hydrostatic forces combined with semi-ordered inter-flake PET and even metal surfaces, is attractive to produce chips,
interactions, which gradually increases with the slow removal of circuits and transparent electrodes. With the recent discoveries
solvent (Figure 6a).120, 121 Of the various assembly methods, VAF regarding rheological properties and LC behavior of MXene, it is
is the most versatile and widely used due to the wide availability now possible to deposit MXene films with varying thickness (nm
of vacuum filtration set-ups in most laboratories. Another to µm) directly from their dispersions. Examples of commonly
appealing advantage of this approach is that it works for any used coating techniques include dip-coating,145 Meyer rod
MXene dispersions regardless of flake size, concentration, or coating (MRC),138 spin-coating,92 and spray-coating146 (Figure 7,
solvent (provided compatiblityof the chosen membrane filter). Table 1). However, it is worth noting that the rheological
Film thickness, and associated dependent properties

requirements for different coating methods vary greatly. For
(conductivity, capacitance and tensile strength) in VAF films, can example, spray coating of inks at high pressure and fast coating
be also easily controlled by adjusting the concentration or rates can be done for MXene dispersion of any viscosity, while
volume of the starting dispersion.64, 121, 122 The MXene extrusion printing requires inks with high elastic modulus to
dispersion can be also mixed with other nanomaterials or preserve the shape of the patterns and prevent the ink from
polymers (e.g., GO, polyvinyl alcohol, cellulose, polydopamine) relaxing and spreading across the substrate. Although coating
to form composite films in order to improve various mechanical processes are generally simple, the MXene and substrate
properties such as elasticity, flexibility and/or toughness.40, 64, surface interaction must be carefully considered. To achieve
121-124
enhanced MXene-substrate interaction, MXene is typically
However, the scalability of a VAF approach is limited by the dispersed in solvent with similar surface energy to that of the
current dimensions of commercial vacuum-filtration substrate.
equipment. Therefore, a scalable method for free-standing film Dip coating (Figure 7a) is a simple method for immobilizing
production is highly desired to eliminate the inherent variation nanomaterials into thin coating layers.145, 147 Here, the
in VAF batch processing. Recently, continuous uniform thin- deposition of thin MXene layers (from ten to a hundred nm)
films up to 1 m in length (~5 cm width) have been fabricated onto a substrate surface relies mainly on the polar nature of its
through a process of blade-coating (BC) (Figure 6b). Unlike VAF, surface terminations, enabling electrostatic self-assembly of
which relies on gravity to stack MXene flakes, BC uses shear flakes onto hydrophilic materials such as glass, 145, 147 PET145, 147
forces to induce flake alignment in an LC-MXene dispersion. and nylon.145, 147 In order to deposit MXene onto hydrophobic
Acquired through proper tuning of rheological properties (zero- substrates, an additional surface treatment method, such as
shear viscosity of >1,000 Pa s and G’/G” > 1), the application of oxygen plasma93 or piranha solution148-150 treatment, is usually
shear force to LC-MXene dispersion aligns MXene flakes along carried out on the substrate to promote MXene adhesion.
the film plane. Using this approach, the voids and spaces Thickness of the coating can be controlled through varying the
present in typical VAF films, which subsequently lowers concentration of the dipping solution, or by prolonging the
conductivity and tensile strength of the MXene architecture, substrate soak time. Using dip coating, production of
were eliminated. The resulting films, with highly aligned and conductive films ranging from 10 nm to 90 nm we realized.
densely stacked MXene flakes (Figure 6b) display exceptional Aside from achieving low resistance (0.08 to 2 k Ω and excellent
tensile strength (~570 MPa) and high electrical conductivity capacitance (1500 F cm-3), these thin films were also found to
(~12,300 S cm-1), which is 25- and 2.3-fold higher than possess high transparency (from 38 to 88% transmittance),
previously reported binder-free films, respectively (Table 1).59 allowing them to be suitable materials for transparent
Owing to their higher conductivity and ordered structure, the electrodes.93, 148, 150 Alternatively, modified dip-coating method
reported EMI shielding efficiency (47.9 dB) of BC films (940 nm- called layer-by-layer (L-b-L) assembly can be utilized. In this
thick) exceed the performance of any other thin-films of method, a thin layer of MXene (few tens to hundreds nm in
comparable thickness to date.59 The mass normalized shielding thickness) can be deposited through electrostatic assembly of
effectiveness of BC films (~1.2 × 105 dB cm2 g−1) was also higher oppositely charged polyions through electrostatic interactions
than most MXene-based films and rivals the highest reported and adsorption, wherein the outermost layer of the film
value for a MXene foam 60 times as thick (~1.3 × 105 dB cm2 dominates the surface charge and characterizes the specific
g−1). This progress notable due to the scalability of BC hydrophilicity or hydrophobicity of the coating.151, 152 Using this
fabrication, which may facilitate the industry-scale production approach, conductive films (~up to 20 S cm-1) with recoverable
of EMI shielding surfaces for future electronic applications. resistance response to bending (~2.5-mm bending radius) and
However, this method is only known to effectively work at a stretching (~40% tensile strain), were produced by alternately
relatively high MXene concentration (>20 mg mL-1), even when dipping low-viscosity MXene and a positively charged polymer,
using large flakes (>10 µm). Production of large MXene flakes at poly(diallyldimethylammonium chloride) (both at ~1.0 mg mL-1)
this concentration is still difficult for most laboratories. The high onto flexible substrates such as poly(dimethylsiloxane), nylon
packing density achieved in the resulting film structure also fiber, glass, and silicon.136 Similar to typical spray-coating
compromises ion transport, resulting in poor electrochemical methods, L-b-L assembly is easily scalability as it doesn’t require
properties.9, 92 highly concentrated MXene dispersions.

Table 1. Summary of conductive MXene films in recent literature. REVIEW
MXene Mechanical
Fabrication Thickness Conductivity
Type of Film loading Strength Notable Properties Ref.
method [µm] [S cm-1]
[wt. %] [MPa]
Vacuum
assisted- 121
~ ~3.3 ~22 ~2,400 ~
filtration
10 | J. Name., 2012, 00, 1-3

(VAF)
(Supercapacitor)
123
VAF ~ ~ ~39 ~4,600
s−1
Gravimetric capacitance ∼330 F g−1 at 2 mV
(Supercapacitor)
125
VAF ~ ~ ~ ~4,400 Gravimetric capacitance ~299 F g-1 at 10 mV
s−1
(Supercapacitor)
Volumetric capacitance ~ 633 F cm-3 at 2 126
VAF ~ ~ ~ ~0.0063
mV s-1
Energy density ~ 41 Wh L−1
(Supercapacitor)
PleaseMaterials
127
VAF ~ ~1 to 21 ~ ~up to 1,250 Areal capacitances ~ 340 mF cm−2 at 0.25
mA cm−2
do not adjust
(Gas Separation)
Horizons
Pristine Ti3C2Tx 128

VAF ~ ~ ~51 ~ H2 permeability >2200 Bar
H2/CO2 selectivity >160

margins
129
VAF ~ ~1 ~ ~14,000 ~
(Lithium Storage/Batteries)
VAF followed Gravimetric capacitance ~ 33 mA h g−1 at 130
~ ~1.94 ~ ~2,800
by annealing 0.05 A g−1
Capacitance retention ~15 % at 4 A g−1
(EMI Shielding/Radiofrequency
VAF followed
identification) 93
by annealing ~ ~0.1 to 8 ~ ~up to 8,000
Reflection coefficient of ~65 dB
Reading distance ~ 8 m at 860 MHz
VAF
(EMI Shielding)
(Proton acid 131
~ ~6-8 ~112 ~10,400 Shielding effectiveness up to ~60 dB
induced self-
Shielding efficiency up to 1600 dB cm2 g−1
assembly)
(Supercapacitor)
79
Spin-coating ~ ~ ~ ~9,880 Aerial capacitance ~1.6 mF cm−2 and energy
DOI: 10.1039/D1MH00968K
View Article Online
density 0.05 µW h cm−2 at 2 mV s−1
This journal is © The Royal Society of Chemistry 20xx

Materials Horizons

Page 10 of 28
Page 11 of 28
Table 1. (continued)
(Transparent Electrodes)
132
Spin-coating ~ ~0.08 ~ ~6,500 Transmittance >97% of visible light per-
Materials Horizons
nanometer thickness
Intraocular lenses (IOL)
Sheet resistance ranging from 0.2 to 1.0 kΩ
133
Spin-coating ~ ~ ~ ~ sq-1
with 50-80% transmittance in the
visible region
(Supercapacitor)
Areal capacitance of ~27 mF cm-2 and 134
Spray-coating ~ ~3 to 6 ~ ~2,500

Volumetric Capacitance of ~357 F cm-3 at 20
mV s-1
Liquid crystal (LC) Blade-coating (EMI Shielding) 59
~ ~0.94 ~570 ~12,300
Ti3C2Tx MXene process Shielding effectiveness up to ~48 dB
Sequentially-bridged (EMI Shielding)
135
Ti3C2Tx VAF 80 % ~5 ~436 ~3,000 Shielding efficiency up to
(alginate and Ca2+) 58,929 dB cm2 g-1
PleaseMaterials
(Supercapacitors)
Sequentially-bridged
Volumetric capacitance ~ 1220 F cm-1 (3- 64
do not adjust
Ti3C2Tx VAF 95 % ~1 ~339 ~4,850

electrode), and ~340 F cm-1 (2-electrode
Horizons
(polydopamine and Ca2+)

device)
(EMI Shielding)

margins
Bridged Ti3C2Tx 95% ~6-7 ~237 ~5,100 124

VAF Shielding effectiveness up to
(poly(dopamine)) 90% ~6-7 ~310 ~4,400
58.4 dB at 8.2 GHz for 95% Mxene
(Supercapacitor)
121
VAF 90 % ~3.9 ~30 ~224
MXene/PVA-KOH composite film at 2 mV s-1
Volumetric capacitance ∼530 F cm-3 for
Ti3C2Tx/ Polyvinyl alcohol (Flexible/thin dielectrics and charge

(Ti3C2Tx /PVA) storage)
129
VAF 10 % ~1 ~ ~ Dielectric permittivity (ε′) ~ 3166
Dielectric loss (tan δ = ε″/ε′) ~ 0.09
(EMI Shielding)
Polyvinyl alcohol/ Layer-by-
~2.72 to ~138 to Shielding efficiency up to 24 550 dB cm2 g−1 39
montmorillonite/ Ti3C2Tx layer 45.5 % ~0.53 to 1.25
8.16 225 Sheet resistance from 855 Ω sq−1 to 3.27 kΩ
(PVA-MTM-Ti3C2Tx) assembly
sq−1
J. Name., 2013, 00, 1-3 | 11

DOI: 10.1039/D1MH00968K
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REVIEW

REVIEW
Ti3C2Tx / (Strain Sensing)

poly(diallyldimethylammo Layer-by- Recoverable resistance response to 136
~ ~ ~ ~20
nium) chloride (PDAC) layer bending (up to 2.5-mm bending radius)
assembly and stretching (up to 40% tensile strain)
(Supercapacitor)
12 | J. Name., 2012, 00, 1-3

Gravimetric capacitance of 324 F g-1 at 10 12
Ti3C2Tx /Glycine VAF ~ ~ ~ ~3,700
mV s-1
(Supercapacitor)
Gravimetric capacitance ~ 326.1 F g−1 at 0.1
A g−1
Aerial capacitance ~ 1.64 F cm−2 at 1 mA
Ti3C2Tx/ Metal Porphyrin 137
VAF 50 to 88.9 % ~16 to 29 ~ ~10 to 1,200 cm−2
Frameworks
Volumetric capacitance ~ 694.2 F cm−3 at 1
mA cm−3
Cyclic stability ~ 30 000 cycles
Areal energy density ~ 20.4 µW h cm−2
PleaseMaterials
Ti3C2Tx / acetylene
Rod Coating (Supercapacitor) 138
do not adjust
black/polyvinylidene 80 % ~125 ~ ~
(on paper) Aerial capacitance ~25 mF cm-2
Horizons
fluoride

margins
(Supercapacitor)
1
Alternate-VAF 95 % ~2 to 3 ~ ~189 to 385 Volumetric capacitance
~ 390 F cm −3 at 2mV s-1
Spin-spray
layer-by-layer
Ti3C2Tx/carbon nanotubes
Assembly
(multi or single-walled) ~0.17
(SSLbL) 4.18 %
(Ti3C2Tx/MW or SWCNTs) (MWCNT)
PVA and (1 MXene : (EMI Shielding) 139
~25 ~Up to 130
poly(sodium 9.38 PVA :1 Shielding efficiency up to 58 187 dB cm2 g−1
~0.27
4- CNT :12.5 PSS)
(SWCNT)
styrenesulfon
ate) (PSS) as
binder
(EMI Shielding)
Ti3C2Tx /Sodium Alginate 37
VAF 10 to 90 % ~1.5 to 45 ~ ~0.5 to 3,000 Shielding effectiveness up to
(Ti3C2Tx/SA)
90 dB (45 µm films)
DOI: 10.1039/D1MH00968K
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Materials Horizons

Page 12 of 28
Page 13 of 28
Ti3C2Tx /Calcium Alginate (EMI Shielding)

140
(Ti3C2Tx/CA) VAF 90 % ~26 ~ 338 Shielding effectiveness ~54.3 dB
Materials Horizons
Shielding efficiency ~17586 dB cm2 g−1

VAF +
electrostatic
assembly (Supercapacitor)
poly(diallyldi
~1,200 to 123
methylammo 90 to 99 % ~ ~ 2mV s-1)
3,300
Volumetric capacitance ∼1040 F cm−3(at
nium) 61% capacitance retention at 1 V s−1

Ti3C2Tx/reduced graphene
chloride energy density of 32.6 Wh L−1

oxide (Ti3C2Tx/rGO)
(PDDA) as
binder
(Lithium Storage/Batteries)
VAF followed Gravimetric capacitance ~ 335.5 mA h g−1 at 130
~ ~ ~18 to 48 ~4 to 67
by annealing 0.05 A g−1
Capacitance retention ~30% at 4 A g−1
PleaseMaterials
(EMI Shielding)
VAF 90 % ~47 ~44 ~7.5 Shielding efficiency up to 2647 dB cm2 g−1
141
do not adjust
50 % ~ ~135 ~0.096 (for 90 % MXene)

Horizons
Alternate-
vacuum
(EMI Shielding)
filtration; 83.3 % ~ ~98 ~25

margins
Shielding effectiveness up to
(Sandwiched) 83.3 % ~ ~95 ~5 142
Ti3C2Tx/Cellulose 30 to 40 dB
(Mixed)
Nanofibres (Ti3C2Tx /CNF)
(EMI Shielding)
VAF 40 % ~38 ~212 ~28 Shielding effectiveness up to 143
39.6 dB
(Supercapacitor)
VAF Gravimetric capacitance of 298 F g−1 (for
80 % ~ ~341 ~295 122
80% MXene)
VAF/
42.86 % (Supercapacitor)
Ti3C2Tx/Bacterial Cellulose Kirigami
(0.75 MXene : ~3 ~70 ~190 Aerial capacitance of 111.5 mF cm−2 144
(Ti3C2Tx /BC) Patterning
1 BC)
(Nanofluidic osmotic power generators)
Ti3C2Tx/Kevlar VAF 89 % ~4.5 ~101 ~ 40
Power Density ~ 4.1Wm−2
J. Name., 2013, 00, 1-3 | 13

DOI: 10.1039/D1MH00968K
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REVIEW

PleaseMaterials
View Article Online

DOI: 10.1039/D1MH00968K

Fig.7. Methods for coating MXene onto surfaces. a) Dip coating of MXene onto glass substrate. Adapted with permission.145 Copyright © 2018 Wiley-VCH, b) Meyer rod coating
process to prepare paper-based supercapacitors. Adapted with permission.138 Copyright © 2016 Wiley-VCH, c) Spin coating of MXene for fabricating transparent electrodes, Adapted
with permission.132 Copyright © 2016 Wiley-VCH, d) Typical schematic of propelling MXene onto desired substrates using spray-gun. Adapted with permission.146 Copyright © 2017
American Chemical Society
MRC, or bar coating, is also a simple, low cost, accessible gold and alumina) coated with a very thin layer of MXene have
and scalable (size and coverage) coating method which has been demonstrated as a broadband absorber for wireless-
been widely used in the manufacturing of conductive screens transmission (WIFI antenna).93 Through spin-coating, LC MXene
and displays for flexible devices.153, 154 MRC uses wire windings dispersions can also be aligned orthogonal to the substrate
attached to a stainless steel rod as an applicator to uniformly surface to form unidirectional pathways, ideal for ion
spread the dispersions into onto the substrate. Similar to BC, transport.92 Compared to horizontally arranged flakes which
application of shear of a viscous MXene dispersion (same possess a tortuous path, the faster transport route enables
viscosity range as BC) allows alignment and dense stacking of thickness-independent electrochemical performance in films,
MXene within the architecture (Figure 7b).138 Film thickness can with 200 F g-1 observed for electrodes with a thickness up to 200
be controlled by adjusting the distance between the wire µm.92
windings, with denser windings resulting in thinner coating. Spray coating, where a material is propelled through a
Using this approach, foldable MXene-on-paper supercapacitors stream of gas or compressed air to be deposited with the aid of
with an areal capacitance of ~25 mF cm-2 were fabricated by a spray gun or atomizer on a given substrate,160 can also be used
coating a MXene/acetylene black/polyvinylidene fluoride slurry to form thin MXene films (Figure 7d). Among several types of
(80:10:10 weight ratio) onto commercial printing paper.138 spray coating methods, (i.e., thermal, plasma, air-gun spray
However, despite being economically promising, only a small methods), the air-gun spray method is the commonly used for
number of studies have employed MRC to fabricate MXene- spray-coating MXene, as it is the least oxidizing.160 146 In contrast
coated surfaces due to the high thickness of the prepared films to dip and rod coatings, MXene coatings with thickness ranging
(typically µm-thick vs. nm-thick coatings for BC) and the from few hundred nm up to few µm can be achieved even by
considerable surface defects and scratches caused by the using regular-sized MXene (<1 µm) at low concentrations (~0.18
interaction of the coated materials with the wire windings.155 mg mL-1).25 Spray-coated films have also been found to have
For spin coating, a certain volume of concentrated MXene properties suitable for surface enhanced Raman scattering
dispersion is placed onto a flat substrate mounted on a disk (SERS) substrates.146 However, these films often form “coffee
which is rotated axially, distributing the solution evenly across rings” or patterns left by droplets of a particle dispersion after
the surface though centripetal shear forces (Figure 7c). The solvent evaporation resulting in uneven coating. To overcome
thickness of the film is determined by the duration and this limitation, dispersions can be mixed with surfactants or
magnitude of the shear force applied, which is proportional to polymer stabilizers, such as ethyl cellulose (similar to spray-
the rate of rotation.156 As an example, ordered, lamellar MXene coated graphene), which enhances MXene adhesion with the
flakes (few nm thick) were deposited parallel with respect to the substrate.161 However, one drawback of this approach is that
plane of polyetherimide substrates through spin-coating a 0.2 the introduction of polymers compromise electrical
mL MXene dispersion (100 mg mL-1, average flake size of~1 µm) conductivity and specific capacitance of MXene.28, 64
at a speed of 1,000 RPM for 60 s.132 The uniform stacking and
alignment of MXene flakes in these films resulted in electrical Prints and patterns
conductivity of 6,500 S cm-1 at > 97% transmittance of visible MXenes’ excellent colloidal stability and tuneable viscosity
light per-nm thickness, surpassing the conductivity of other makes them particularly suitable as inks for printing and
equivalent solution-processed 2D material transparent films (> patterning. Though the major drawback of most printing
97% trans.). These substrates supported electrodes have been methods is the high viscosity requirement, the recent progress
readily integrated into microelectronic, photonic integrated on LC-MXenes makes high viscosity inks achievable at lower
circuits, and silicon photonic devices, for a wide range of MXene concentrations. MXenes are also redispersible in a wide
applications from optical sensing to light detection and variety of aqueous and organic solvents, without the addition of
telecommunications.157-159 Plasmonic substrates (e.g., glass, surfactants or stabilizing agents whose residue may

Horizons
compromise the electronic properties of the films. Aside from > Gʺ) at low shear stress (<100 Pa), to solidify the MXene
View ink
Article Online
simply using MXene dispersions as inks in ball-point pens for during the screen-printing process. Screen-printing of MXene is
DOI: 10.1039/D1MH00968K
directly writing circuit patterns and designs (Figure 8a),162 low-cost and scalable, and the thickness of the printed patterns
typical pre/post-patterned coating162 and printing95 are simple, can be tuned by controlling the concentration or aspect ratio of
economically efficient, versatile, and eco-friendly the MXene flakes. The main drawbacks of screen-printing
manufacturing techniques for MXene incorporated devices. however, are low resolution, high roughness, and the high ink
Printing techniques can be generally divided into digital (inkjet viscosity required resulting in low scalability.164, 166
printing) and non-digital (direct writing, screen and transfer Lastly, inkjet printing (Figure 8d) is a versatile method that
printing), with screen and inkjet being the main MXene printing involves a limited number of process steps, is amenable for
methods used. These different printing/coating techniques mass production, and can deposit controlled amounts of
typically differ in ink rheological property requirements, material. Typically, inkjet printing requires ink viscosity within a

resolution, and scalability, allowing researchers to choose a narrow range (~1 to 20 MPa s), which is easily achievable for
suitable method for the criteria met by their MXene dispersions. MXene dispersions with concentration ~1 to 5 mg mL-1 (for
Transfer printing and/or stamping involves transferring flakes ~1 to 3 µm wide).26, 59 Inkjet printing has been recently
material from relief features on an intermediate medium onto used to directly print a flexible MXene-films onto a various of
the target substrate using a paint roller or through stamping substrates such as PET,95, 167 cellulose paper,167 and glass.167
(Figure 8b).163 This method enables quick and simple These films when fabricated into supercapacitors demonstrate
heterogeneous integration of different classes of materials into excellent electrochemical performance, including volumetric
desired layouts, especially for the production of capacitance up to ~560 F cm−3 and energy density as high as
flexible/stretchable electronics. However, for effective printing, ~0.32 µW h cm−2. Likewise, inkjet printed films possess
MXene with high viscosities ranging from 50 to 1,000 MPa s excellent conductivities (~1000 S cm-1) resulting in high energy
(concentration of ~3.5 to 30 mg mL-1 for dispersions of MXene shielding efficiency with values reaching 50 dB at films with
flakes with size of ~1 µm) must be used to ensure that the ink thicknesses of ~1.35 µm.
can be stamped or rolled.59, 162, 163
Screen printing on the other hand, works by depositing Fibers and yarns
materials though squeezing high-viscosity inks via a stencil The recently growing trend towards portable and wearable
screen onto a substrate (Figure 8c).165, 166 In this approach, the devices has placed new demands on fibers, such as the ability
viscoelastic behavior of MXene must be tuneable through shear to conduct electricity,168 harvest and store energy,11, 26, 94, 169, 170
rate adjustment, where the high viscosity ink must show liquid- and sense motion.15, 115, 168 Such demand has led to the
like behavior (dominant Gʺ) at high shear stress (>500 Pa), development of a new generation of “multi-functional
allowing it to be smoothly extruded through the screen mesh to fibers”.171 These fibers are typically assembled by incorporating
the substrate, while still retaining the printed structure after highly conductive, energy storing, and mechanically strong
deposition.164, 166 The ink must then possess elastic behavior (Gʹ materials, including polymers such as poly(3,4-
Fig 8. Methods for printing MXene patterns onto surfaces. a) Direct writing of patterns using a pen injected with MXene ink. Adapted with permission.162 Copyright © 2018 WILEY-
VCH Verlag GmbH & Co. b) Transfer printing using concentrated MXene stamping ink. Adapted with permission.163 Copyright © 2018 WILEY-VCH Verlag GmbH & Co. c) Screen
printing of complex patterns using MXene/polymer ink formulations. Adapted with permission.164 Copyright © 2020 Wiley-VCH. d) Inkjet printing using a MXene ink dispersed in
an organic solvent. Adapted with permission.164 Copyright © 2020 Wiley-VCH

PleaseMaterials
ethylenedioxythiophene):poly(styrenesulfonate),169 rGO,100, 172 and amines, enhancing adhesion between the flakes andOnline
View Article the
and nanoparticles such as colloidal silver.173 In this section, an substrate. Of the various fibre substrates cotton
DOI: based fabrics
10.1039/D1MH00968K
overview on the current methods in processing MXene interact particularly well with MXene,175, 176 for example,
dispersions into fibers and yarns is summarized (Table 2) along MXene-coated cotton fibres were acquired through a two-step
with discussion on how these methods are influenced by the dip-coating method where the internal yarn structure was
colloidal and rheological properties of MXene dispersions.25, 27 infiltrated with small MXene followed by coating large MXene
Coating MXene on existing fibres and yarns. Like film flakes (concentration of ~10 to 15 mg mL-1) on the yarn surface
substrates, MXene flakes can be also coated onto individual (Figure 9a). This strategy maximized both conductivity and
fibers, twisted yarns, and knitted or woven fabrics thereby flexibility, and showed minimal changes in resistance and
introducing electrical conductivity, electrochemical behavior MXene mass loading after a series of washing cycles (MXene
and other desirable properties such as EMI shielding. This loading ~77 wt% or ~2.2 mg cm−1 and conductivity ~440 S cm−1)

approach has been commonly used for both natural (e.g., (Figure 9a). However, more than 10 successive dip coating
cotton,174-176 linen,176 and bamboo176) and synthetic fibers (e.g., cycles (approximately 12 h) is required to functionalize a yarn of
nylon,175 polyester,177 and carbon fibers94). While the usual limited length (2 m), making the process time intensive for
coating process of soaking the fibres in a dispersion of MXene is practical commercialization.175 The inherently strong adhesion
simple, the surface chemistry and morphology of the fiber- of MXene onto cotton and nylon allowed the development of
based substrate plays a critical role in the adhesion between an automated coating process where commercial yarns were
MXene flakes and fibre surface. It has been known that all passed through successive baths of MXene (150 µm) each
negatively charged MXenes,178 can interact well with followed by drying.175 This method led to large scale production
hydrophilic or positively charged substrates, and particularly (spools of > 10 m length) of MXene fibers with a mass loading
those containing hydroxyl or amine functional groups. Features of up to 51 wt.% and a resistance of ~8.4 Ω at 1 cm.
which are commonly present in most natural and synthetic Meanwhile, surface functionalization and addition of
fibers. Aside from these electrostatic interactions, the presence chemical adhesives to substrates were also explored to coat
of transition metals in the structure of MXene may also result in MXene onto chemically inert fibers (e.g., carbon fibers) (Figure
the coordination with functional groups such as carboxylates 9b). These methods include oxygen plasma treatment, 179
addition of conductive polymer binders (e.g., PEDOT:PSS),94 as
well as surface functionalizations or grafting (e.g.,
silanization).177 As an example, one of the earliest works
exploring MXene as a coating was MXene-modified carbon fibre
supercapacitor with a length capacitance of ∼130 mF cm−1,
fabricated using MXene (20 mg mL-1) as an active material and
PEDOT-PSS (4 mg mL1) as binder. The addition of the conductive
binder enabled MXene adhesion to the carbon fiber substrate,
functionalizing this inherently inert material.94
Trapping and/or Spinning MXene into fibres and yarns.
MXene can be also incorporated within a fiber structure by
adding MXene dispersions into material formulations (e.g.,
spinning dopes) for use in fiber production through methods
such as biscrolling,170, 180 electrospinning61, 181, 182 and wet
spinning.61, 181, 182 In this section, details of commonly used fiber
processes are reviewed in terms of how the MXene dispersions
were utilized and introduced into formulations.
Biscrolling is a fibre fabrication method that involves twist-
based spinning of CNT flakes (as host) that are overlaid with a
layer of up to 99 weight percent (wt %) of other functional
materials (as guest).180 This method is usually employed to turn
the guest nanomaterials, which are often unspinnable (e.g., low
viscosity MXenes), into scroll-shaped CNT-supported yarns
(Figure 10a). The introduction of guest nanomaterials onto
drawn CNT flakes is usually achieved through drop-casting,180
in-situ deposition,183 or dip-coating184 prior to the
twisting/spinning of the CNT forest. Although the particles are
Fig 9. MXene-coated fibers. a) MXene-coated cotton yarns. A two-step coating
process involving an initial coating of small MXene large MXene flakes to maximise
trapped within scroll corridors of the CNT host, these remain
both yarn flexibility and conductivity. Adapted with permission.176 Copyright © 2019 electrochemically accessible due to the loose-stacking and small
Wiley-VCH., b) MXene/PEDOT:PSS formulations coated onto chemically inert carbon diameter of the CNTs that comprise the thin scrolls. Biscrolled
fiber yarns (scale bar = 10 μm). Adapted with permission.94 Copyright © 2017 Royal
Society of Chemistry

Table 2. Electrical, mechanical, and electrochemical properties of selected MXene-based fibers, yarns, and fabrics in the current literature
Page 17 of 28
Notable properties
Ref.
Linear
MXene Strain- Volumetric Areal Gravimetric
Materials Horizons
Type of Fiber Method Tensile capacitanc

loading Diameter Conductivity to- capacitance capacitance capacitance
strength e
[μm] [S cm-1] failure Cv Ca Cg
[MPa] CL
[%] [F cm-3] [mF cm-2] [F g-1]
[mF cm-1]
MXene-coated MXene 176
Coating ~610 ~200 ~460 ~10 ~0.26 ~3,965 ~ ~760
cotton yarn (78 wt.%)
MXene
MXene/silver- 179
Coating (0.7 mg ~500 ~ ~ ~ ~ ~328 ~ ~50
coated nylon yarn
cm-1)

MXene /poly(3,4-
MXene,
ethylenedioxythio
PEDOT:PS
phene):
S 94
polystyrene Coating ~120 ~200 ~3,000 ~1.6 ~ ~659 ~30 ~252
(1.8 mg
sulfonate
cm-1
(PEDOT:PSS)-
MXene)
coated carbon tow
PleaseMaterials
MXene-coated MXene
199
carbonized silk Coating (2 mg cm- ~ ~ ~ ~ ~ ~362 ~ ~
2)
fabric
do not adjust
MXene
Horizons
MXene-coated 200
Coating (2.6 mg ~ ~ ~ ~ ~ ~416 ~200 ~
carbon fiber fabric
cm-2)

margins
MXene
MXene-coated 175
Coating, knitted (~22.5 ~ ~ ~ ~ ~ ~707 ~31 ~566
cotton knit fabric
mg cm-2)
MXene,
Biscrolled MXene/ CNT
170
carbon nanotube Biscrolling (~97 ~120 ~ ~37 ~15 ~1,100 ~3,200 ~523 ~118
(CNT) yarn wt.%
MXene)
MXene,
Biscrolled MXene/
CNT 201
carbon nanotube Biscrolling ~56 ~2.7 ~38 ~5 ~92 ~ ~ ~
(95 wt.%
(CNT) yarn
MXene)
MXene,
carbon
MXene/carbon fiber 61
Electrospinning ~ ~ ~ ~ ~ ~244 ~110 ~
fiber mat (~22
wt.%
J. Name., 2013, 00, 1-3 | 17

DOI: 10.1039/D1MH00968K
View Article Online
REVIEW
MXene)

REVIEW
MXene,
MXene/ carbon CNT
nanotube (CNT) @ (21.5 202
Electrospinning ~ ~ ~3 ~97 ~ ~50 ~100 ~
polycaprolactone wt.%
(PCL) fiber mat MXene/C
18 | J. Name., 2012, 00, 1-3

NT)
MXene/ polyester MXene,
191
(PET)/silver- Electrospinning PET ~ ~ ~ ~ ~ ~72 ~ ~
coated nylon yarn (~)
MXene/ poly(3,4- MXene,
ethylenedioxythio PEDOT 169
Wet-spinning ~ ~1,500 ~60 <2 ~615 ~676 ~258 ~4.6
phene (PEDOT) (70 wt.%
fiber MXene)
MXene,
MXene/ reduced
rGO (88 203
graphene oxide Wet-spinning ~70 ~70 ~130 ~3 ~341 ~233 ~257 ~1.2
wt.%
(rGO) fiber
MXene)
MXene,
MXene/ reduced
PleaseMaterials
rGO (90 198

graphene oxide Wet-spinning ~25 ~290 ~13 ~4 ~891 ~565 ~495 ~
wt.%
(rGO) fiber
MXene)
do not adjust
MXene,
Horizons
MXene/
PCL 28
polycaprolactone Wet-spinning ~130 ~0.002 ~4 770 ~ ~ ~ ~
(30 wt. %
(PCL) fiber

margins
MXene)
MXene/polyureth MXene,
115
ane (PU) coaxial Wet-spinning PU ~50-100 ~10-5 ~40 ~400 ~ ~ ~ ~
fiber (~1 wt.%)
MXene
26
LC-MXene fiber Wet-spinning (100 ~45 ~7,750 ~40 1.7 ~1,300 ~1,762 ~393 ~
wt.%)
MXene
105
LC-MXene fiber Wet-spinning (100 ~40 ~7,700 ~60 0.22 ~ ~ ~ ~
wt.%)
MXene
MXene from 104
Wet-spinning (100 ~12 ~12,500 ~340 0.28 ~ ~ ~ ~
deformable ‘gel’
wt.%)
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Materials Horizons

Page 18 of 28
Horizons
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DOI: 10.1039/D1MH00968K

Fig 10. Free-standing MXene fibers. a) MXene/CNT yarns made using biscrolling. Adapted with permission. 170 Copyright © 2018 Wiley-VCH. b) MXene/Carbon fiber mat acquired
from carbonizing electrospun MXene/PAN fibers. Adapted with permission.181 Copyright © 2020 Wiley-VCH. c) MXene composite fiber made from a solution of MXene and
PEDOT:PSS processed through vertical wet-spinning. Adapted with permission.169 Copyright © 2019 Wiley-VCH. d) Neat fibers from wet-spinning of additive-free LC-MXene
dispersions. Adapted with permission.26 Copyright © 2020 American Chemical Society.
MXene-CNT yarns, were demonstrated through drop casting MXene/alginate,182 and MXene/PAN61. However, it is known
dilute dispersions of MXene in DMF (2 mg mL-1) onto stacks of that the intercalation of polymers between MXene reduces
CNT forests that are subsequently twisted into a helical yarn inter-flake contact resulting in loss of conductivity.28, 64 It is also
(Figure 10a).170 SEM images of the yarns revealed that MXene known that electrospinning high mass loading of very
flakes were trapped within the CNT network through the conductive materials like MXene, is challenging due to the
formation of helical yarn corridors. The resulting architecture excess charges in the polymer jets that dissipate quickly to the
also possessed varying sized pores and voids allowing collector plate inducing opposite charges on collector resulting
infiltration by aqueous electrolytes, giving specific capacitance in lifting off of the deposited fibres.192 In addition, high loading
as high as ~1,100 F cm−3 (~3,200 mF cm−2), with energy (61.6 of conductive fillers in the spinning dope increases the
mWh cm−3) and power densities (5,428 mW cm−3) exceeding solution’s conductivity, often resulting in short circuiting and
previously recorded capacitance for any yarn supercapacitor even flashover under high voltage. In this regard,
electrode. However, the drawback preventing scale-up and electrospinning is usually limited to spinning dopes with
commercialisation is high cost of the CNT forests, limited length relatively low MXene content (<1 wt. %).
of yarns, and the known bio-safety issues of CNTs in wearable To overcome this inherent limitation and fabricate highly
devices raising health and safety concerns.180, 185-187 Efforts to conductive MXene electrospun fiber mats, a subsequent
minimize these hazards include functionalization of CNTs with a carbonization step of MXene/PAN can be carried out to
protective polymer for improved biocompatibility188 or transform the polymer into graphitic carbon, thereby gaining
encapsulation of the device with polymer/resin to prevent electrical conductivity.61 Other works include electrospinning
nanomaterial exfoliation.189 MXene/PEO fibers and incorporating them into polyester yarn
The dispersibility of MXene into a wide variety of polar coated with thin layer of conductive Ni-Cu alloy.191 However,
solvents have made them ideal additive materials for these studies only used a relatively small amount of MXene (<
electrospinning. In a typical electrospinning set-up, a material 35 wt.%) in the spinning dopes, therefore desired properties
(e.g., conductive polymer) is extruded from a syringe capped such as volumetric capacitance were not maximized. In another
with a needle, to which high voltage is supplied, opposite a work, a nylon/PU dope was electrospun into a bath of MXene
grounded metal collector, either a metal plate or a roller, onto to achieve a fibrous mat up to ~90 wt% MXene, with high
which the fiber mat is collected.61 Several works have notably electrical conductivity (~1,200 S cm−1)(Figure 10b).181 This
used electrospinning to produce MXene composite fiber mats, approach effectively captured MXene flakes continuously along
including MXene/chitosan,190 MXene/polyethylene oxide the nylon/PU nanofiber yarns, enabling utilization of MXene’s
(PEO),182, 191 MXene/polyvinyl alcohol MXene/ (PVA),182 electrical and electrochemical properties, offering an innovative

PleaseMaterials
alternative method to produce conductive fibrous mats and properties, and processing of pure MXene fibers are Online
View Article still
membranes required. A recent innovation in spinningDOI:
of pure MXene fibers
10.1039/D1MH00968K
Wet-spinning is an efficient way to produce long functional includes the induced gelation of spinning dopes using NH4+ as
fibers, as demonstrated by the scalable production of the coagulation bath to increase the packing of flakes through
conductive polymer,193 CNT,98, 194 and graphene fibers.172, 195-197 electrostatic and Van de Waals interactions.104 Fibers acquired
In this method, a spinning solution, typically polymer dissolved though this method exhibit a 1.5-fold increase in electrical
in solvent, is injected through a spinneret into a solvent bath conductivity (12,500 S cm−1) and Young’s modulus (120 GPa)
that results in coagulation of the polymer into a fiber (Figure compared with previously reported pure MXene fibers.
10c). The continuously produced fiber is subsequently removed
from the bath, washed, dried, and collected onto a winder. Three-dimensional (3D) MXene architectures
An effective strategy to realize spinnability of MXene

Apart from processing into compact structures (films and
suspensions is to combine MXene with inherently spinnable fibres), several techniques have also been recently reported to
polymers or nanomaterials to form composite fibers. Due to the produce MXene-based 3D architectures with interesting
excellent dispersibility of MXene in a wide variety of polar macroscopic architectures resulting in high porosity that are
solvents, a large range of materials, e.g. polycaprolactone suitable for a range of practical applications such as energy
(PCL),28 PU,115 PEDOT:PSS,169 and graphene oxide,198 have been storage and catalysis. The following section of this review
used as matrices of MXene-based composite fibers with loading focuses on the progress in preparing 3D foam-like (sponge or
ranging from 10 to 98 wt.%198. Similar to previously discussed aerogel) MXene-based materials. Here, their chemical
techniques, simple variation in MXene content in the spinning composition/structure as related to material properties is
solution results in the modulation of mechanical strength, described to provide a rational and in-depth direction for the
electrical conductivity and electrochemical performance to development of MXene-based 3D architectures.
match the target application. As an example, a report on wet- MXene-Coated foams. The template method to produce
spun MXene/PU composite fibers that possess both high foams uses an inherently porous template on which MXene
conductivity and high stretchability, at a very low percolation flakes can be easily deposited. For instance, a thin layer of
threshold (~1 wt. %), have demonstrated excellent strain chitosan (CS) on PU sponge can provide a positively-charged
sensing performance.115 This fiber exhibits a high gauge factor surface enabling electrostatic attachment of negatively-charged
(GF) of ~12,900 (~240 at 50% strain) and a large sensing strain MXene (at concentrations < 10 mg mL-1). MXene is simply
of ~152% demonstrating the viability of wet-spinning coated on the template using dip-coating, or L-b-L assembly
elastomeric composites to achieve MXene-based strain sensing (Figure 11a).204 These fabricated MXene/CS-coated PU sponges
fibres and textiles suitable for applications in health, sports, and demonstrate high reversible compressibility (of up to 85%), with
entertainment. good structural stability. However, most of this aerogel is
However, varying the spinning formulations properties (e.g., composed of PU foam (both wt. and vol. %), resulting in lower
density and rheology), modifications in the spinning set-up, energy density and conductivity. Therefore, methods that
coagulation bath, and post-treatments are generally required. utilize active porous materials that interact favourably with
For example, spinning MXene/PEDOT:PSS fibers into a sulfuric MXene such as preformed rGO aerogels205 and Ni foams206 have
acid bath where upward injection of the spinning dope is been explored as template materials (Figure 11b). The surface
required due to the higher density of the bath relative to the of rGO aerogels possess abundant H-bonding sites arising from
injected solution (Figure 10c).169 In a further example, carboxylate and ether functionality on which the MXene surface
MXene/GO fibers required a chemical reduction process after termination can interact (Figure 11c). When used as an
spinning to reduce the GO and recover the electrical electrode, this porous MXene-coated RGO aerogel displayed
conductivity.198 Another option to simplify MXene spinning both high specific capacitance (~130 F g-1) and energy density
conditions is to directly spin fibres from pure MXene (~35 Wh kg-1) with capacitance retention of 95% after 75,000
dispersions. With the recent discoveries on the LC behavior of charge-discharge cycles. Meanwhile, the Ni foams provide
MXene, pure MXene fibres can now be also produced through active metallic surfaces that can readily form coordinate
shear-induced alignment of LC phases in a typical fibre wet- covalent bonds with MXene terminations. Due to the
spinning process (Figure 10d).26 Here, MXene flakes are highly conductive substrate, the resultant 3D composite gave
aligned along the fibre axis, resulting in excellent electrical excellent conductivity, exhibited a high specific capacitance
conductivity (∼7,750 S cm−1) and volumetric capacitance (654 F g-1 at 1 A g-1) and good cycling stability (80% capacitance
(∼1,300 F cm−3). This combination of excellent electrical and retention after 5000 cycles). However, despite these works
electrochemical properties enabled the production of demonstrating quick and simple MXene functionalization of 3D
prototype MXene fiber-based supercapacitors and textile architectures, by only relying interaction between surface
heater.26 Such devices only required a low power density of terminations the MXene coating is vulnerable to exfoliation.
∼126 W cm−2 at an applied voltage of 24 V, to reach a Freeze-dried aerogels. The vulnerability of MXene
temperature of 68 °C.26 However, these fibres continue to exfoliation and the low MXene loading achieved through dip-
display poor tensile strength due to the loose MXene packing coating porous templates is the common drawback of coating
and the presence of micro/macro structural voids. Thus, further
research in improving strength, discovering other new

Horizons
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DOI: 10.1039/D1MH00968K

Fig 11. MXene Aerogels acquired through coating porous template/support with MXene. a) MXene/CS coated PU sponge acquired through repeated dip-coating. Adapted with
permission.204 Copyright © 2019 Elsevier Inc. b) Preparation of MXene-coated rGO aerogel, Adapted with permission.205 Copyright © 2019 Wiley-VCH., and c) L-b-L MXene coating
of Ni foam using CTAB as counter-electrolyte. Adapted with permission.207 Copyright © 2019 Elsevier Inc
methods discussed in the previous section. Therefore, (Figure 12). GO flakes and carboxylate functionalized CNTs are
alternative strategies producing MXene-embedded porous 3D very hydrophilic, can be easily dispersed in high aqueous
architectures have been explored. Recently, ultra-low density concentrations and have strong π-π stacking, making them ideal
pure MXene aerogels (<10 mg cm-3) have been fabricated from precursors for strong and flexible aerogels.213, 215, 216 Such
freeze-drying dispersions. (<1 µm, < 10 mg mL-1).208 properties also make them suitable MXene scaffolds, with
Unfortunately, the weak gelation capability of pure MXene resulting aerogels possessing aligned cellular microstructures,
results in deficient aerogels, with low elasticity and irreversible where the stacked MXene/rGO213 or MXene/CNT215 assemblies
compressibility. To address these drawbacks, the addition of act as shells of the aerogel cell walls, resulting in excellent
fillers and bridging agents such as organic molecules (e.g., electrical conductivity (9.43 S cm-1 for MXene/CNTs)215.
cellulose,209, 210 chitosan,204 polyimide,211 and alginate212) and 3D printed architectures. The recently growing
other nanomaterials (e.g., rGO)213, 214 into the MXene solution understanding in the rheological properties of MXene inks
before solution processing into composite aerogels. The as- (Section 3.3) also gave rise to the 3D printing of foams and other
obtained freeze-dried aerogels exhibited interconnected porous 3D structures (i.e., electronic chips, micro-
networks formed through covalent cross-linking and/or supercapacitors etc.) (Figure 13).217, 218 High concentration (50
hydrogen-bond interactions between MXene and the polymer. mg mL-1) aqueous inks were prepared from LC-MXene (8 µm)
These aerogels also possess good reversible compressibility, which possessed elastic modulus and yield stress of ~36,500 and
stretchability, and excellent fatigue resistance (e.g., up to 1000 ~200 Pa, respectively, within the range for printable inks
cycles at 50% strain for the MXene/rGO aerogel).213, 214 reported for other polymer-based systems. 3D-printing of
However, again the addition of polymer additives results in a MXene architectures can serve as a scalable approach to
drastic > 10-fold decrease in electrical conductivity due to the fabricate custom-shaped MXene-based integrated devices. As
reduction in inter-flake contact. One alternative strategy is the an example, a custom-shaped, ready-to-use supercapacitor
addition of nanomaterial fillers such as GO (consequently
reduced to rGO)213, 214 and CNTs215 into the MXene dispersion

PleaseMaterials
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DOI: 10.1039/D1MH00968K

Fig 12. Freeze-drying method of fabricating MXene-based aerogels. A schematic illustrating the MXene aerogel fabrication process through freeze-drying using rGO as
nanomaterial filler. Adapted with permission.214 Copyright © 2018 American Chemical Society.
Fig 13. 3D printed MXene architectures. A schematic illustrating the manufacturing strategy developed for 3D printing of freestanding MXene architectures starting from the
synthesis of MXene up to the fabrication of the MSC device. Adapted with permission.217 Copyright © 2019 Wiley-VCH.
which achieved a high areal capacitance value of 2,100 mF cm−2 Although a huge variety of processing methodologies have been
and gravimetric capacitance of ~242 F g−1 with 90% retention developed, significant challenges and opportunities still exist before
even after 10,000 charging/discharging cycles has been MXene architectures can be fully realized in practical applications.
assembled through 3D printing. The resulting device exhibited Like other nanomaterials,6, 220 challenges on translating the
high energy density of 0.0244 mWh cm−2 and a power density nanoscale properties of MXene into the macroscale architectures
of 0.64 mW cm−2 at a current density of 4.3 mA cm−2.219 that simultaneously display outstanding mechanical, electrical and
Although only used as proof-of-concept demonstrations, the electrochemical properties are yet to be fully addressed. The trade-
method of 3D-printing MXene structures offers an exciting offs in these properties in MXene composites are caused by either
innovation towards the design of intricate architectures (e.g., one, or a combination of, 1) small flake size and magnified defects
3D circuits/symmetric capacitors, Figure 13) that cannot be
(per flake area), 2) isotropic arrangement of MXene flakes resulting
easily produced by other fabrication methods.
in void formation, misalignment and irregular stacking of MXene
flakes, 3) poor inter-flake connectivity, and 4) reduced accessibility
Outlook in achieving optimal MXene properties and architectures
to electrochemically active sites due to MXene aggregation. Based
As discussed in this article, a great number of studies have been on these challenges, the following techniques have provided
dedicated towards improving the conventional methods of essential solutions in addressing the gaps in both material synthesis
processing MXene into functional architectures. To summarise, the and processing which thereby significantly contribute to the advance
fabrication process typically starts from choosing an ideal etching of the practical application of MXenes.
procedure, in order to acquire MXene flakes with desired properties.
Producing large flakes with minimal defects
Deeper understanding on fundamental properties such as
rheological and LC behavior of such MXene dispersions has provided
Only a small number of studies have demonstrated the use of
crucial information on finding the suitable processing strategies on
exceptionally large MXene flakes (~15µm) in fabricating functional
which a certain MXene dispersion can be fabricated with optimal
architectures.26, 59, 104, 105 However, the advantages of maximizing
functional material properties for a targeted practical application.
flake size is proven to be two-fold. First, it enables long-range

Horizons
ordering of MXene flakes, achieving nematic LC phases at a very low inter-flake interactions are sufficiently weak.221 TheseView
methods are
Article Online
Ct. This allows easier manipulation of ordered LC phases in various attractive in achieving well-aligned architectures since they offer
DOI: 10.1039/D1MH00968K
processing architectures to yield highly ordered structures, resulting clean, contact-free, mechanical stress-free or electrostatic charge-
in improved mechanical strength. Second, ultra-large flakes showed less methods, which works equally well for thin films and bulk
very minimal basal and edge defects relative to surface area, samples.222-226
translating the excellent properties inherent in single flakes into
device performance. Although a few interesting reports on this topic Designing MXene interfaces
have been undertaken, a more detailed correlation of the LC
Finally, we believe that tuning the surface properties of MXenes
behavior and the rheological properties is still needed to enable the
would also serve a crucial role to further progress the already rapidly
preparation of appropriate LC-MXene dispersions for the desired
growing field of MXene architecture fabrication. The negatively

solution-based processing technique.
charged surface of MXenes (zeta potential of around -40 mV) allows
However, during this early stage in the development of MXenes, them to form highly stable colloidal dispersions in water, thereby
acquiring large and defect-free flakes has proven difficult due to the resulting in their versatile solution processability. MXenes also retain
hazards imposed by harsh synthetic procedures. Likewise, the this negative surface charge in a wide pH range (from ~4 to 12),
additional process of sonication to delaminate the flakes introduce providing opportunity for surface modification in various solvent
further structural damage to the MXene flakes. Methods which avoid environments. Early methods of MXene surface modifications
the use of sonication and unwanted intercalants, such as the MILD include mixing MXene with cellulose nanofibers,122, 141 alginate,135, 140
method, have made it possible to acquire large single layer MXene and montmorillonite,39 which are linked by non-covalent interactions
flakes (> 10 µm) with minimal structural defects. Applying the “junk- such as hydrogen bonds and electrostatic forces. Innovations in non-
in-junk-out” principle (i.e., large starting materials lead to large covalent functionalization such as the recently reported sequential-
products) in these methods has further increased the acquired flake bridging methods,64, 135 which entails a two-step non-covalent
sizes to >15 µm, much larger than in previous reports, by size- functionalization (e.g., MXene H-bonding with a polymer fortified
selecting >40 µm MAX from the highly polydisperse starting through cationic cross-linkers) has proven to significantly improve
material.59 However, MXene flakes with dimensions >20 μm have yet the performance of MXene films (e.g., improved mechanical strength
to be demonstrated. The acquisition of such “ultra-large” flakes without the compromise in conductivity and capacitance).
through these modified synthetic procedures is believed to play a Meanwhile, only a few studies on covalently bonded surface
crucial turning point in developing the scaled-up fabrication of functionalization of MXenes have been demonstrated, but they
improved MXene architectures such as BC films or wet-spun fibers. provide interesting information towards tuning the properties of
MXene dispersions and architectures. For example, functionalization
Manipulating flake alignment with [3-(methacryloxy)propyl]trimethoxysilane enabled MXene to be
dispersed in non-polar solvents for the first time.227 Meanwhile Cl-
While problems concerning selecting large flake size and minimizing and Br-terminated MXenes, which are capable of halide ion exchange
structural defects could be addressed during synthesis (above), the for specific atoms and functional groups, can provide precise control
other factors such as voids, orientation and packing density were on tuning the surface chemistry of MXene materials.26
found out to be addressed by the choice of assembly process. For
example, the BC method which uses shear to induce flake alignment Aside from opening new functions for MXene, this capability to
(Figure 3b), has produced films with higher degree of anisotropy functionalize and selectively tune the surface terminations could
(assessed using Herman’s orientation factor, (f)) compared to the potentially lead to enhance compatibility towards a larger variety of
commonly used VAF for making MXene films. The shear-induced surfaces and substrates thereafter limiting the problems of
assembly also allowed the deposition of evenly spaced flakes with delamination such as in the case of coatings. From another
minimal voids, resulting in excellent conductivity and EMI shielding perspective, these surface modification methods would not only
performance (~12,000 S cm-1 and ~50 dB respectively). Although, not enable tunability of colloidal stability of MXene on a wider variety of
yet demonstrated for other MXene architectures (e.g., fibers and solvents but would consequently provide potential coupling sites for
aerogels), it is expected that the optimized alignment of flakes could enhanced inter-MXene flake connectivity. The resulting material
also adapted into modified fiber-spinning methods (i.e., increased would possess improved mechanical properties of pure MXene
shear rate to promote flake alignment) and lyophilisation process of architectures even without the addition of a polymer matrix, which
producing aerogels (i.e., size and directionality driven by flake is crucial for the scalable and practical use of MXene-based
dimensions). Since most MXenes display metal-like electrical architectures.
conductivity, the application of electric fields could also open new
avenues in tuning their behavior in solution for manipulating their Conclusion
morphology and properties during the fabrication of MXene
In recent years, we have witnessed the booming MXene research in
assemblies. This method has yet to be shown for MXene but has been
a wide range of applications ranging from energy
demonstrated in graphene oxide LCs such that macroscopic
generation/storage, EMI shielding, wireless communications
alignment could be controlled even at low electric fields so long as

PleaseMaterials
catalysis, gas/molecule adsorption, and many more. We envisage 11. S. Seyedin, E. R. S. Yanza and Joselito M. Razal, J. Mater.
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that incorporating the above principles to current material Chem. A, 2017, 5, 24076-24082. DOI: 10.1039/D1MH00968K
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Gao and Y. Chen, Carbon, 2009, 47, 922-925.
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expected that the continuously growing knowledge in this exciting Y. Chen, Chem. Soc. Rev., 2015, 44, 647-662.
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innovations in design principles and fabrication methodologies will J. M. Razal, Mater. Horiz., 2019, 6, 219-249.
pave the way for other types of MXenes and even to the larger family 16. M. Naguib, M. Kurtoglu, V. Presser, J. Lu, J. Niu, M. Heon,
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18. G. Deysher, C. E. Shuck, K. Hantanasirisakul, N. C. Frey, A.
Author Contributions C. Foucher, K. Maleski, A. Sarycheva, V. B. Shenoy, E. A.
Stach, B. Anasori and Y. Gogotsi, ACS Nano, 2020, 14, 204-
K.A.S.U, D.Y.H and J.M.R. conceived and outlined the review.L.C.H, S.Q. 217.
and J.Z contributed in writing and editing several sections in the review. 19. B. Anasori, Y. Xie, M. Beidaghi, J. Lu, B. C. Hosler, L.
All authors discussed and revised the manuscript. Hultman, P. R. C. Kent, Y. Gogotsi and M. W. Barsoum, ACS
Nano, 2015, 9, 9507-9516.
20. A. Shayesteh Zeraati, S. A. Mirkhani, P. Sun, M. Naguib, P.
Conflicts of interest V. Braun and U. Sundararaj, Nanoscale, 2021, 13, 3572-
3580.
There are no conflicts to declare. 21. T. S. Mathis, K. Maleski, A. Goad, A. Sarycheva, M. Anayee,
A. C. Foucher, K. Hantanasirisakul, C. E. Shuck, E. A. Stach
and Y. Gogotsi, ACS Nano, 2021, 15, 6420-6429.
Acknowledgements 22. M. R. Lukatskaya, S. Kota, Z. Lin, M.-Q. Zhao, N. Shpigel, M.
The authors acknowledge the financial support from the D. Levi, J. Halim, P.-L. Taberna, M. W. Barsoum, P. Simon
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Ti3C2Tx MXene: From Dispersions to Multifunctional Architectures for

Article in Materials Horizons · August 2021

Ken Aldren Sumaya Usman Si Qin

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Luke C Henderson Jizhen Zhang

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Ti3C2Tx MXene: From Dispersions to Multifunctional Architectures

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MXenes, Ti3C2Tx has been the most studied, possessing

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Ken Aldren S. Usman is a PhD Dylan Y. Hegh is currently a

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Table 1. Summary of conductive MXene films in recent literature. REVIEW

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Pristine Ti3C2Tx 128

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density 0.05 µW h cm−2 at 2 mV s−1

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Ti3C2Tx VAF 95 % ~1 ~339 ~4,850

(polydopamine and Ca2+)

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Bridged Ti3C2Tx 95% ~6-7 ~237 ~5,100 124

Ti3C2Tx/ Polyvinyl alcohol (Flexible/thin dielectrics and charge

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Ti3C2Tx / (Strain Sensing)

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