Ceramics International 47 (2021) 4398–4403

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Ceramics International
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Review article

Fabrication strategies and application fields of novel 2D Ti3C2Tx (MXene)

composite hydrogels: A mini-review
Qinhua Wang a, 1, Xiaofeng Pan b, 1, Xinpin Wang a, Shilin Cao a, Lihui Chen a, Xiaojuan Ma a, *,
Liulian Huang a, **, Yonghao Ni a, c, ***
a
College of Material Engineering, Fujian Agriculture and Forestry University, No. 15 Shangxiadian Road, Cangshan District, Fuzhou City, Fujian Province, 350002, PR
China
b
Centre for Energy, Materials and Telecommunications, Institut National de la Recherche Scientifique, 1650 Boulevard Lionel-Boulet, Varennes, Québec, J3X 1S2,
Canada
c
Limerick Pulp and Paper Centre, Department of Chemical Engineering, University of New Brunswick, Fredericton, New Brunswick E3B5A3, Canada

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

Keywords: Ti3C2Tx (MXene), a new kind of 2D ceramic nanosheets, is receiving more and more attention in the fields of
Ti3C2Tx (MXene) medicine, biology, energy, electronics, etc. However, the preparation and application of MXene in hydrogel is
Hydrogel still in its infancy period. Here, we review the latest progress (after 2018) related to MXene hydrogels in time.
Dispersibility
Aiming at the key issue of the dispersion stability of MXene in hydrogel systems, the preparation strategy,
Self-assembled
Conductive
mechanism, advantages and disadvantages of MXene hydrogels are sorted out in detail, and the potential
Photothermal application prospects of MXene composite hydrogel are introduced. Finally, future viewpoints are put forward
for the dispersion stability challenges that need solving in the design of MXene hydrogel.

1. Introduction interference shielding (EIS), to wearable electronics fields [11]. There­

The Ti3C2Tx (MXene), transition metal carbides, nitrides, and car­
bonitrides, a class of 2D nanomaterials, which was first introduced by
the Gogotsi group in 2011, has recently set off a multidisciplinary
research boom [1,2]. Interestingly, it has many similarities in structure
and performance with 2D graphene nanosheets. Therefore, given its
high conductivity, mechanical rigidity, photothermal conversion effect,
antibacterial ability, high specific surface area, and outstanding volu­
metric capacitances, it has abundant applications in the fields of batte­
ries, capacitors, electromagnetic shielding, photothermal agents,
sensors, etc [3–7]. However, previous studies have mostly focused on
MXene in other materials (aerogels, membranes, and rubber compos­
ites), and the preparation and application of MXene composite hydro­
gels are rather limited [8–10]. In fact, the hydrogel substrate provides a
great and versatile platform for MXene nanosheets. In particular,
MXene-based hydrogels have significant unique and enhancing attri­
butes from energy storage, catalysis, tissue engineering, electromagnetic
fore, MXene-based hydrogels have huge potential for further exploration
in future research and development.
It is well known that MXene has good dispersibility in water solvents
due to its hydrophilic surface groups (-OH, –O, -Ti, -Cl, and –F) [12–14].
Regrettably, MXene tends to self-aggregate in aqueous media through
vdW attraction and hydrogen bonding [15,16]. Therefore, the nano­
sheets accumulation is likely to occur during the hydrogel fabrication
period, which affects the preparation of a uniform MXene hydrogel [17].
In addition, nanosheets are also prone to deposition and oxidation in
as-prepared hydrogels, greatly affecting the comprehensive perfor­
mance of hydrogels [18]. Although recent reviews detailed the con­
struction of various 3D assemblies of MXene, those MXene hydrogels are
scarcely covered, and they are limited to self-assembled MXene gels [19,
20]. There are still shortcomings in the collection of extensive MXene
hydrogel preparation methods and applications. Herein, we organize
this mini review in time to review and analyze previous MXene com­
posite hydrogel preparation strategies and introduce potential

* Corresponding author.
** Corresponding author.
*** Corresponding author. College of Material Engineering, Fujian Agriculture and Forestry University, No. 15 Shangxiadian Road, Cangshan District, Fuzhou City,
Fujian Province, 350002, PR China.
E-mail addresses: 1212juanjuan@163.com (X. Ma), fafuhll@163.com (L. Huang), yonghao@unb.ca (Y. Ni).
1
Q.W. and X.P. contributed equally to this work.

https://doi.org/10.1016/j.ceramint.2020.10.096
Received 22 August 2020; Received in revised form 5 October 2020; Accepted 13 October 2020
Available online 14 October 2020
0272-8842/© 2020 Elsevier Ltd and Techna Group S.r.l. All rights reserved.
Q. Wang et al.
applications of MXene composite hydrogels. For MXene hydrogel design
and application, some feasible approaches and timely reminders are
proposed.
2. Synthetic strategies of MXene composite hydrogels
In Fig. 1a, the multilayer MXene was synthesized via etching out the
Ti3AlC2 MAX phase with hydrogen fluoride [14]. The multilayer MXene,
which has an accordion-like structure, is very unstable in aqueous sol­
vents (Fig. 1b) [21]. The oligolayer MXene obtained by ultrasonic
peeling and centrifugal treatment of multilayer MXene will have better
water dispersion stability (Fig. 1c), so it is usually applied for the
preparation of composite hydrogels [15]. Nevertheless, the preparation
of the oligolayer MXene composite hydrogel still needs to consider the
stability of the MXene nanosheets in the water solvent and as-prepared
hydrogel (Fig. 1d) [15,22]. We have compiled the following strategies
for the preparation of MXene hydrogels, which may solve this puzzle and
simultaneously promote the synergistic improvement effect of nano­
sheets on the hydrogel system. The following describes in detail the
fabrication strategies of oligolayer MXene composite hydrogel (MXene
composite hydrogel for short) fabrication (Table 1).
2.1. MXene-doped thickened polymer hydrogels (class I)
Here, the fabrication strategy of MXene composite hydrogel is
introduced, by mixing MXene with a thickened polymer solution (high-
viscosity solution), and then self-assembling with a crosslinker for
preparation. For instance, Zhang et al. incorporated MXene into
Fig. 1. a) Preparation strategies for common oligolayer MXene nanosheets. Reproduced with permission [14]. Copyright 2019, Wiley-VCH. b) SEM images of MAX,
multilayer MXene, and oligolayer MXene nanosheets. Reproduced with permission [21]. Copyright 2019, American Chemical Society. c-d) Digital pictures of oli­
golayer MXene suspension. Reproduced with permission [15]. Copyright 2019, American Chemical Society.
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Ceramics International 47 (2021) 4398–4403
polyvinyl alcohol (PVA) solution, and then used borax cross-linking to
prepare self-healing MXene-PVA hydrogel (Fig. 2a) [23]. Xing et al.
added MXene into cellulose solution to finally prepare MXene-cellulose
hydrogels with photothermal effects [21]. Furthermore, the Alirez group
also tried to introduce 2D MXene in a honey-chitosan mixture and then
cross-link to prepare a biocompatible MXene-honey-chitosan hydrogel
[24]. Generally, the thickened polymer has a large viscosity, which can
prevent the re-stacking of the MXene nanosheets, so the dispersion
stability of the hydrogel can be improved. However, due to the strong
binding effect between thickened polymers, it is also difficult for MXene
to connect uniformly among polymer networks [25].
2.2. MXene nanosheet/small molecule self-assembled hydrogels (class II)
Recently, researchers have proposed a novel strategy for in situ self-
assembly of MXene nanosheets and small molecules to form a hydrogel.
For instance, Deng et al. mixed a metal ion (Fe2+, Mg2+, Co2+, Ni2+, and
Al3+) with MXene suspension, and the self-assembled hydrogel quickly
formed through the connection of ions and –OH surface of MXene at
room temperature (Fig. 2b) [26]. In addition, under the action of
reducing agents (L-Cysteine,EDA,NH3⋅H2O, N2H4⋅H2O), the mixed so­
lution of MXene and graphene oxide (GO) can form a self-convergent
MXene/GO self-assembled hydrogel after high temperature treatment
[27]. This strategy facilitates the formation of great physical and
chemical bonding between small molecules and MXene nanosheets, that
is, MXene is the backbone of the hydrogel, so the stability of the nano­
sheets in the hydrogel greatly improves [28]. However, some of the
above-mentioned hydrogel preparation processes need to endure high
Q. Wang et al. Ceramics International 47 (2021) 4398–4403

Table 1
Summary of MXene hydrogel products.
Composition Type Preparation Preparation Stability Mechanical property Conductivity Photo Application Year Ref.
time temperature (Max) -thermal

MXene/cellulose I ＞1.5 h 65 ◦ C Moderate Compressive – Yes Photothermal 2018 [21]

strength therapy
34.7 kPa
MXene/PVA I ~5 min 20 ◦ C Moderate ＞3400% Yes – Sensor (GF:25) 2018 [40]
MXene/PVA I ＞9.5 h 90 ◦ C Moderate ≈1200% Yes – Sensor (GF:0.40) 2019 [23]
MXene/honey/ I ~1 h 37 ◦ C Moderate – Yes – Cell attachment and 2020 [24]
chitosan survival
MXene/metal ion II ~1 min 20 ◦ C Great Storage modulus: Yes – Supercapacitor 2019 [26]
7 kPa electrodes (at 226 F
g− 1 at 1 V s− 1)
MXene/GO/EDA II ＞6 h 95 ◦ C Moderate Storage modulus:15 Yes – Supercapacitor 2019 [27]
kPa electrodes (at 370 F
g− 1 at 5 A g− 1)

MXene/PNIPAM III ＞24 h 20 ◦ C general Young’s modulus： – Yes Photothermal 2018 [30]
8.66 kPa response smart
switch
MXene/PNIPAM/ III ＞24 h 10 ◦ C general Up to 1400% 1.092 S/m – Sensor 2019 [32]
PAM

MXene/PAM III – 20 ◦ C great Up to 3047.5% – – Drug release 2020 [33]

MXene/PNIPAM III Few minutes 20 ◦ C great Storage modulus:3.5 0.019 S/m Yes “Smart” window 2019 [34]
kPa

MXene/PVA/ I/ ＞6 h 90 ◦ C Moderate Up to 1200% Up to 4.25 S/m – Sensor (GF:44.85) 2019 [31]

PAM III

PVA—Polyvinyl alcohol; GO—Graphene oxide; EDA— ethylenediamine; PNIPAM—Poly(N-isopropylacrylamide); PAM— Polyacrylamide.

“-“: Not available or not mentioned in references.

temperature treatment for a long time, which may oxidize the MXene
nanosheets and finally affect the hydrogel performance. Moreover, the
ion-crosslinked MXene composite hydrogel has poor stretchability,
which may limit its durability [29].
2.3. MXene nanosheet induced polymer composite hydrogels (class III)
Mixing 2D MXene and monomers to form in-situ polymerized
MXene-polymer hydrogel is also one of the common MXene-bases
hydrogel fabrication strategies. In this strategy, MXene nanosheets
mainly play the following three roles.
In the first category, MXene is incorporated into gel systems as nano
reinforcers or functional nanomaterials (eg, conductive agents and
photothermal agents). For example, Yang et al. dispersed MXene
nanosheets in NIPAM (monomer) solution and then polymerized and
crosslinked to prepare near-infrared-responsive MXene-PNIPAM
hydrogels (MXene as photothermal agent) [30]. Liao et al. and Zhang
et al. incorporated MXene nanosheets into a dual-network polymer
hydrogel system, which simultaneously acted as the hydrogel’s
conductive agent and nano reinforcers [31,32]. Unlike thickened poly­
mer solutions, this type of monomer solution has low viscosity. There­
fore, the easy aggregation of MXene during long-term hydrogel
manufacturing needs to be emphasized.
In the second category, MXene suspensions have clay-like properties,
so MXene can be employed as a crosslinker for polymer hydrogels. For
instance, Zhang et al. applied MXene nanosheets as a crosslinking agent
to obtain MXene-PAM nanocomposite hydrogels (Fig. 2c) [33]. In this
system, the reducing surface of MXene can activate the initiator through
the redox reaction, thereby rapidly generating many hydroxyl radicals
(⋅OH) to promote the polymerization of the monomers [28]. At the same
time, MXene can quickly cross-link polymer chains to form
self-assembled nanocomposite hydrogels. Here, MXene nanosheets
greatly improve the speed of hydrogel fabrication and finally prevent the
accumulation of nanosheets during the preparation period. In addition,
MXenes are well locked by polymer chains as crosslinkers, so they are
difficult to deposit in the as-prepared hydrogel.
The third category introduces MXene as a monomer reaction plat­
form to prepare polymer hydrogels. Recently, Tao et al. discovered that
sonicated Mxene can autonomously generate ⋅OH radicals, and then
initiate the self-polymerization of different monomers (including
acrylamide AM, DMA, MMA, HEMA) with ultrafast speed (Fig. 2d) [34].
At the same time, MXene, which is the starting point of the polymeri­
zation of the monomers, can assemble the polymer chains to form a
MXene/polymer hydrogel. Like the second category, the preparation of
this type of MXene hydrogel is very fast, and the nanosheets also have
great stability in the hydrogel system.
3. The application of MXene composite hydrogels
The 2D MXene nanosheets have various great properties, such as
electrical conductivity, nano-reinforcement, photothermal properties,
and antibacterial properties [35]. Next, we discuss the role of MXene in
composite hydrogels and the application of hydrogels tuned by MXene.
For instance, the MXene can absorb near-infrared and convert it into
thermal energy, so MXene doped hydrogel can be used as a carrier of
photothermic agent [33,36]. Xing et al. demonstrated MXene/cellulose
hydrogel can be used for photothermal therapy (PTT) in vivo (Fig. 3a)
[21]. In addition, MXene/PNIPAM hydrogels were fabricated using
MXene in combination with temperature-sensitive polymers, which can
change the transparency of the hydrogel by near-infrared light and apply
it to smart windows (Fig. 3b–c) [34]. Similarly, by adjusting the
macroscopic morphology of the gel in the near infrared, MXene/PNI­
PAM hydrogels can be also used for light-controlled microfluidic pipe­
line switches (Fig. 3d) [30]. Here, the uniform and stable distribution of
the MXene can promote the response stability of hydrogel smart devices.
Moreover, like most nanoparticles, MXene nanosheets can signifi­
cantly improve the mechanical properties of composite gels through the
bond action of nanosheets and polymers. For example, Zhang et al.
added MXene to a PAM hydrogel system to increase the extension ratio
of the composite hydrogel to 30 times that of pure PAM hydrogel
(Fig. 3e) [33]. Combined with the high conductivity of MXene
(6000–8000 S cm− 1) (Fig. 3f), MXene composite hydrogel is suitable for

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Fig. 2. Various synthetic strategies of MXene composite hydrogels. a) Schematic presenting the synthesis of the MXene-doped thickened PVA hydrogel. Reproduced
with permission [23]. Copyright 2019, Wiley-VCH. b) Schematic of the MXene/Fe2+ self-assembled hydrogel. Reproduced with permission [26]. Copyright 2019,
Wiley-VCH. c) Fabrication procedures of MXene/PAM hydrogels by free radical polymerization with MXene nanosheets as a crosslinker. Reproduced with permission
[33]. Copyright 2020, Royal Society of Chemistry. d) Schematic illustration of MXene-initiated polymerization and subsequent gelation. Reproduced with permission
[34]. Copyright 2019, Royal Society of Chemistry.

preparing stretchable hydrogel sensors and electronic skin. Zhang et al.
realized the handwriting and human expression recognition by
MXene-PVA hydrogel (Fig. 3g–h) [23]. The stable dispersion of MXene
nanosheets in the gel system has a significant effect on improving the
conductivity and mechanical strength of hydrogel.
The rich surface groups of MXene nanosheets also provide good
reactivity, so it can be used as an in-situ polymerization platform for
polymer hydrogels as an alternative crosslinker and initiator. More
importantly, Deng et al. demonstrated that MXene/metal ion self-
assembled hydrogel can effectively avoid the restacking of MXene
nanosheets, which greatly improves its surface utilization rate, and has
high rate performance when used as a supercapacitor electrode (Fig. 3i)
[26]. In addition, the in-situ assembled polymer hydrogel of MXene
synthesized by our group also demonstrates great anti-oxidation ability,
which is mainly due to the protective effect of polymer chains on its
edges. Therefore, the resultant hydrogel can be applied as a stable
moist-electric nanogenerator for power generation [18]. In addition,
unlike graphene, MXene can have both high reactivity and conductivity
(for electron transport). When MXene nanosheets are assembled into
hydrogels, the performance as catalyst support will be improved [11].
Importantly, the design and regulation of the MXene nanosheets on the
oxidation degree, as well as the influence of its interactions with other
components of the gel system on the photocatalytic performance, should
be further studied [37]. In fact, MXene hydrogels have been less
explored in the photocatalysis field, and are expected to warrant more
research activities in the future.
In summary, the outstanding talent of MXene needs to be reasonably
utilized to prepare hydrogels that meet the needs of specific fields. At the
same time, the fabrication approach of the MXene composite hydrogel
needs to be further designed to improve the dispersibility of the nano­
sheets and the performance and stability of the gel products [38,39].

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Fig. 3. a) Cell viabilities of HepG2 after different contents of MXene hydrogel treatments. Reproduced with permission [21]. Copyright 2019, American Chemical
Society. b) Transmittances of MXene/PNIPAM hydrogel as a function of temperature. Inset shows the thermo-responsiveness of the hydrogels. Reproduced with
permission [34]. Copyright 2019, Royal Society of Chemistry. c) Application of MXene/PNIPAM hydrogel for simulated “smart” window. Left: before irradiation.
Right: after irradiation. Reproduced with permission [34]. Copyright 2019, Royal Society of Chemistry. d) Liquid microvalves fabricated by the MXene/PNIPAM
composite hydrogel. The photographs show the microvalve before (top) and after (bottom) exposure to NIR irradiation. Reproduced with permission [30]. Copyright
2018, Royal Society of Chemistry. e) Mechanical behaviors of as-prepared MXene/PAM hydrogels. Reproduced with permission [33]. Copyright 2020, Royal Society
of Chemistry. f) Electrical conductivity of MXene/PAM hydrogel [31]. Reproduced with permission. Copyright 2019, Wiley-VCH. g) SEM images of MXene/PVA
hydrogel surface before and after stretching. Reproduced with permission [40]. Copyright 2018, AAAS. h) Schematic for signature sensing of MXene/PVA hydrogel
sensor. Reproduced with permission [40]. Copyright 2018, AAAS. i) Rate performances of MXene powder and MXene/Fe2+ self-assembled hydrogel at different scan
rates. Reproduced with permission [26]. Copyright 2019, Wiley-VCH.

4. Conclusions and perspectives Declaration of competing interest

Currently, the preparation and application of MXene composite The authors declare that they have no known competing financial
hydrogels are in their infancy period. There are still two major con­ interests or personal relationships that could have appeared to influence
straints in the design and preparation of MXene composite hydrogels. the work reported in this paper.
First, the poor dispersibility of MXene nanosheets in the hydrogel
directly affects the stability, conductivity, mechanical property, etc. of Acknowledgments
the gel. In addition, the rapid oxidation of the MXene in the water sys­
tem of the hydrogel has a great weakening effect on the comprehensive The authors are grateful to the National Key Research and Devel­
properties of the gel, but it is often ignored by researchers. This previous opment Program of China (2017YFB0307900), National Natural Sci­
research demonstrates that the dispersibility of MXene can improve by ence, Foundation of China (31770632), Natural Science Foundation of
rationally modifying the MXene nanosheets. The 2D MXene as a reaction Fujian Province (2015J05093), and the Innovation Fund from Fujian
platform to prepare self-assembled hydrogels may be an alternative Agriculture and Forestry University (CXZX2017296 and
approach to this problem. Moreover, the addition of a reductive sub­ CXZX2017037).
stance and a polyanionic electrolyte proved to achieve stable anti-
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