Emergent Materials

https://doi.org/10.1007/s42247-021-00204-7

REVIEW

MXenes and their composites for hybrid capacitors

and supercapacitors: a critical review
Manavalan Vijayakumar 1,2 & George Elsa 2 & Aamani Nirogi 2 & Rajendran Navaneethan 2 &
Ammaiyappan Bharathi Sankar 3 & Mani Karthik 2

Received: 6 February 2021 / Accepted: 3 March 2021

# Qatar University and Springer Nature Switzerland AG 2021

Abstract
MXenes are realized as an innovative family of two-dimensional (2D) structured materials resembling the structure like graphene
and molybdenum disulfide. The extensive research has been explored in this novel family of MXene materials from the discovery
of Ti3C2 in 2011. Around 20 variants of MXenes have been synthesized, and the structural properties of more than dozens of
MXene materials have been theoretically predicted. Unlike other 2D ceramics, MXenes have excellent electrical conductivity
and exceptional efficiency since they are molecular sheets composed of carbide and transition nitride metals such as titanium.
MXenes are formed by etching a coating from MAX phases and adding the suffix “ene” to highlight their resemblance to
graphene. MAX phases are a family of hexagonal faceted ternary transition metal carbides, carbonitrides, and nitrides composed
of Mn+1AXn, where M represents for transition metals (such as Cr, Nb, Ti, V), A indicates group of A elements (such as In, Al, Si,
Sn), X means carbon and/or nitrogen, and n=1, 2, or 3. MXenes have already established numerous applications such as energy
storage, modular electronics, optoelectronics, medicine, and nano-biosensors. In this review article, the synthesis technique,
configuration, and electronic properties of MXenes are emphasized and extensively discussed. MXenes and MXene-based
nanocomposites for electrical energy storage applications are mainly highlighted and outlined. Finally, MXene-based hybrid
supercapacitors as next-generation energy storage devices are summarized and briefly discussed.

1 Introduction technologies exhibit variable power supply and ambiguous

output. Renewable energy sources like wind and sun are un-
1.1 Concept of energy storage and technology certain energy sources because the wind does not blow con-
tinuously, and the sun does not shine constantly at any given
Sustainable and renewable energy conversion technologies location [2]. There is an urgent need to create a relatively
and their development have become the consensus of scien- constant energy storage device as a crucial component for
tists all over the world. Renewable sources of energy like future powering systems. In the future, the electricity grid
wind, solar, and tidal can minimize the usage of fossil fuels has to include energy storage systems to maintain the uninter-
and reduces the greenhouse gas emissions in power generation rupted power supply to the end consumers [3].
[1]. Solar photovoltaic (PV) and wind energy conversion The power grid is a complex mechanism in which the pow-
er generation and power demand should be balanced at any
given time. The constant supply modifications are needed for
* Mani Karthik predictable power demand shifts, such as normal trends of
mkarthik@project.arci.res.in; karthik_annauni@yahoo.co.in human activity, as well as unpredictable incidents from over-
1
loads of the high-power demand of alternators [4]. Energy
Global Innovative Centre for Advanced Nanomaterials (GICAN), storage plays an imperative role in the balancing act which
Collage of Science, Engineering and Environment, The University of
Newcastle, NSW 2308 Callaghan, Australia also facilitates the development of more sustainable and se-
2 cure grid infrastructure. For example, where there is more
Centre for Nanomaterials, International Advanced Research Centre
for Powder Metallurgy and New Materials (ARCI), Balapur, energy availability than power consumption during the night
Hyderabad 500005, India when low-cost power stations start running, surplus electricity
3
School of Electronics Engineering, Vellore Institute of Technology generation for reserved capacity could be used. When the
(VIT), Chennai Campus, Chennai 600127, India power demand exceeds supply, storage facilities will
 emergent mater.

distribute their stored energy to the reservoir. Energy storage renewable energies, such as solar or wind, and has a major
is awaited to play a huge role in the coming century, with obligation to fulfill potential energy needs [8]. This technolo-
more storage capacity solutions evolving and the transition gy will help to remold the energy sector by integrating renew-
from the planet to a cleaner energy economy. Energy storage able energy sources (solar power and wind) into the utility grid
is also used as a fast solution, and most storage systems will as shown in Fig. 2. It will allow saving the electrical energy by
start to discharge electricity into the grid very rapidly, whereas supporting the sudden power demand variations in balancing
fossil fuel supplies appear to ramp up longer. This rapid re- and maintaining the grid. Globally, there has been a shift to-
sponse is critical to ensure grid reliability when unanticipated wards clean energies with more focus on climate change, and
demand changes occur [5]. there is a gradual transition from fossil fuels to renewable
While considering environmental climate changes and eco- resources. Energy storage traditionally refers to storing elec-
nomic standards, it is important to examine different compet- trical energy previously generated for use at a later time.
ing technologies including generation, transmission, distribu- Simultaneously, energy from renewable sources should be
tion, and operational circumstances. To store energy for a long stored effectively and efficiently in energy storage devices.
period, different energy storage technologies are available in Currently, LIBs contribute a predominant function partic-
the market such as batteries, supercapacitors (SCs), thermo- ularly hybrid electric and various electronic gadgets.
electric, mechanical storage, hydrogen, and pumped hydro- Rechargeable LIBs and SCs are the most beneficial inventions
power [6]. Based on the technology and its application, design for electrochemical energy storage (EES) systems [9]. LIB
considerations and specific factors change for each compo- batteries often carry huge energy densities but offer low power
nent used in the application, i.e., reliability, environmental densities that limit their operation in an environment that de-
impact, and safety. Generally, various energy storage technol- mands more energy. SCs, on the other hand, offer higher
ogies have been developed and demonstrated as illustrated in power densities with outstanding cycling efficiency with low
Fig. 1. The electricity storage systems vary in shape and size energy densities being their liability. As a result, many re-
depending on the type of energy stored which include thermo- searchers around the world are researching new materials of
electric, hydro, gas turbine, flywheel, superconductive mag- excellent energy and power density and are therefore viable
netic coil, SC, lead-acid battery, Li-ion battery (LIB), and fuel over a longer span of existence [10].
cell stacks. To reduce the gap between power demand and Since the finding of exfoliated graphene films in 2004, 2D
availability of electricity, electrical energy storage systems material with a layered structure has appealed to a great re-
tend to reduce scheduling variations [7]. search interest among scientists due to their fantastic electron-
Energy storage is a process that transforms one form of ic and structural properties. After the two decades of the suc-
energy into another form by storing it and using the stored cessful mechanical exfoliation of graphene from three-
energy at a later time. Electrical energy can be derived from dimensional (3D) graphite, several 2D nanomaterials have

Fig. 1 Various technologies of an electricity storage system

emergent mater.

Power Conversion System

Solar Power
Power Transmission

Lead Acid Battery Grid Pack

Hybrid Energy Storage

Variable Power Generation
Stable Power Generation

Supercapacitor Grid Pack

Power Substation
Li-ion Grid Pack
Wind Power
Fig. 2 Integration of renewable energy sources from solar power and wind power to the utility grid

been explored by using different preparation and exfoliation generate a MAX layer of layer and incorporate a suffix called
methods from different layered precursor materials which in- “ene,” which underlines their graphene resemblance. The
clude metal-organic frameworks (MOFs), graphitic carbon MAX phases are a huge group of ternary hexagonal layered
nitride (g-C3N4), and different MAX phase (e.g., Ti2AlC), as transition metal carbides, carbonitrides, and nitrides with a
well as other precursors, which are utilized to obtain the 2D chemical formula of Mn+1AXn, where M is the transition metal
transition metal carbides (TMC), carbonitrides, and nitrides; like Ti, V, Cr, and Nb, where A indicates group A elements
those are generally called “MXene” [11]. such as Al, Si, Sn, and In, X indicates carbon and/or nitrogen,
2D materials could act as fundamental building blocks to and n indicated as n=1, 2, or 3 respectively. The MAX phase
form various layered structures, composites, and membranes. means a variety of metals with Mn+1AXn chemical composi-
Even though some individual 2D elements, such as graphene, tion. The present review article introduces and explores thor-
silicon, germanene, and phosphorene, are synthesized, most oughly the synthesis techniques, structural composition, and
of these materials are comprised of two or more atoms, such as
chalcogenides in metal transition and double-layered hydrox-
ides [12]. Graphene has shown outstanding research potential
in 2D materials and has immense energy conservation and
transformation capacity. For the first time, Gogotsi’s research
group reported the convergence of metallic conductance and
hydrophilic surfaces in a novel constellation of graphene-like
2D compounds, metal transition carbides, carbonitrides, and
nitrides, and this category of 2D material was known as
MXenes [13]. Following this discovery of the MXenes, sev-
eral scholars have researched systematically the design and
production of 2D materials because of their excellent electri-
cal, optical, and mechanical characteristics, which have a high
aspect ratio. Figure 3 indicates that the number of articles
published is related to MXenes and MXenes composites [14].
In particular, MXenes have high electrical conductivity and
outstanding performance as compared to other 2D materials,
since they are molecular sheets crafted from carbides and tran-
sition metal nitrides such as titanium. These types of 2D layer- Fig. 3 The number of articles published each year in the field of MXenes
structured materials are known as “MXenes” since they and MXene-based composites.
 emergent mater.

physicochemical properties of MXenes. Special attention has different structures of one metal at the M-site, as obtained
been given to MXenes and their composite materials for en- from the parent peak phases: M2C, M3C2, and M4C3. They
ergy storage applications. Finally, MXene-based hybrid SCs are generated by carefully inscribing the element A of the
as next-generation energy storage devices are also extensively MAX process or other layered predecessor (e.g., Mo2Ga2C)
discussed. with the structural formula of Mn+1AXn, where M is an early
transition metal, A is an element of the periodic table group 13
or 14, X is C and/or N, and n = 1–4. These are generally
2 Synthesis strategy of MXenes referred to as mono-transition metal MXenes. MXene car-
bides consisting of two transition metals referred to as double
After the identification of peculiar properties of graphene, transition MXenes have also been synthesized [15].
there has been a substantial investigation on 2D materials. In In this latest millennium, MXenes have been standardized
this concern, 2D TMC and nitrides are explored, and it is as M′2M″C2, M′2M″2C3, or M′4M″C4. Mo2TiC2, Mo2Ti2C3,
called as MXenes (pronounced as “Maxenes”) that was steadi- Cr2TiC2, and Mo4VC4 contain synthesized double transition
ly increasing class of 2D materials. MXene is a novel type of metal carbides, where M′ and M″ are different transition
organized 2D material which is similar to that of graphene and metals. Mo or Cr atoms are extreme parts of the MXene such
molybdenum disulfide material. This novel family of MXene as Mo2TiC2, Mo2Ti2C3, and Cr2TiC2, and these atoms are
has been thoroughly investigated in the year of 2011, after the responsible for the electrochemical efficiency of the
discovery of Ti3C2 material. To date, there are around 20 MXenes, while in some of the MXenes like Mo4VC4 or
variants of MXenes that have been synthesized, and their (Mo,V)4C3, the metals are aimlessly dispersed across the sys-
structural and physicochemical properties of more than tem in stable solutions. Generally, MXenes are fabricated by
dozens of MXenes have been theoretically predicted. Also, using different techniques as schematically represented in Fig.
such materials find an extensive potential material in various 5.
applications. The history and evaluation of MXenes are sche- For example, amine-assisted delamination is being a two-
matically represented in Fig. 4. step process and frequently utilized to segregate different lay-
MXene has a standard formula of Mn+1XnTx where Tx ered materials into 2D nanosheet materials [16], which are
indicates the surface circumcisions that are bound to the outer generally obtained through intercalation of an organic com-
M layers (O, OH, F, and/or Cl). MAX phases have a pound into the layered structure followed by sonicating in a
hexagonal-layered configuration in which M layers are virtu- solvent. Dimethyl sulfoxide (DMSO) can act as an intercalat-
ally closed, and octahedral sites are filled by X atoms. Layers ing agent during the synthesis of MXenes [17]. Initially,
of Mn+1Xn are then interlaced with element A, which is me- multi-layered Ti3C2Tx flakes can be delaminated. Afterward,
tallically attached to element M. MXenes also have three the delamination of this same compound could also be carried

Fig. 4 History and periodic assessment of MXene and MXene-based composites for numerous potential applications
emergent mater.

Fig. 5 Various routes for

fabrication of MXenes

out by using a simple etching method of the MAX phase, reaction time, (iv) a 0.2 s Tetrakis (dimethylamino) hafnium
Ti3AlC2, in a solution containing LiF and HCl [18]. On the (Hf(NMe2)4) precursor dose, and (v) a 15 s Hf(NMe2)4 reac-
other hand, the coating of SnO2 and HfO2 with ALD (atomic tion time with a growth rate of 0.1 nm per cycle [18]. ALD
layer deposition) was specifically applied to MXene layers was utilized to implant one single layer of metal carbide
coated on a Cu surface. MXene base can be prepared by using (MXene) onto mTMDC (single-layer transition metal
the mixer of MXene powder, acetylene black, and dichalcogenide) and to eventually oxidize the top layer of
polyvinylidene fluoride (PVDF) with a corresponding weight metal atoms [19]. Spark plasma sintering (SPS) is one of the
ratio of 80:10:10 by adding NMP as a solvent for preparing promising methods owing to its numerous benefits offered
the homogenous mixture. By using a doctor blade instrument, over other MAX-phase preparation techniques. The PL-SPS
the prepared mixture was evenly transposed on a copper foil densification process is similar to the conventional SPS meth-
having a coating thickness of 100μm, and the coated material od, and the transport mechanism is similar to the grain size
was dried at a temperature of 80°C for 24 h under vacuum diffusion. The mechanical compaction is used only relevant to
condition. For SnO2 and HfO2 deposition, the MXene-coated the punches that cause the grain to move the current and the
Cu foil was placed into the atomic layer deposition chamber reaction merging into the grain boundary instead of the fric-
with the measurement of material active mass (1–2 mg cm−2). tion. The spark current flows to punches and finally to the
For example, SnO2 was deposited at two different tempera- sample that is sintered through the electrodes [20]. It is a
tures of around 150°C and 200°C by using an ALD reactor. unique process used to accumulate pressurized powder in
The deposited sample at 150°C was further treated in subse- which pulsed direct electrical current travel through the sam-
quent steps: (i) a constant N2 dose at 20 psi, (ii) a dose of Sn ple and it is pushed through a matrix of graphite. The electric
precursor (Tetrakis (diethylamide) tin (IV)) at 0.5s, (iii) an Sn current sintering is also referred to as the ground-assisted or
precursor reaction time of 30 s, (iv) an O3 oxidant dose at 0.2 pulse-assisted sintering process [21]. The loaded solution is
s, and (v) an oxidant reaction time of 15 s with a deposition then mixed with the sample, and the solvent is evaporated in a
rate of 0.1 nm per stage. The standard cycle at 200°C liquid-phase impregnation process. An impregnation by a for-
contained the same precursors, but the reaction times were mulation with a power sample is equal to the material’s pore
modified to achieve a reasonable thickness of SnO2 MXene volume, and also it is added to the inception of the impregna-
sheets. tion processes [22]. The process of exfoliation applies to the
On the other hand, ultra-thin films of HfO2 were also de- preparation of MXene from the MAX stage (discriminatory
posited at 180°C on the surface of the SnO2/MXene elec- layers of A-group components in the MAX step using HF
trodes. The following steps are involved in the preparation etchant solution) [23, 24].
of HfO2 deposition by using the ALD technique: (i) a constant The synthesis of MXene materials by ball-milling with the
20 psi N2 dose, (ii) a 0.015 s H2O dose, (iii) a 10 s H2O aid of liquid surfactants or solid microdermabrasion additives
 emergent mater.

is a result of high energy colliding nanosized particulates in This process involves mounting and removing surface
balls-milling materials (bulk precursors). The transition of functional groups by replacing and reducing reactions of mol-
metal atoms into the perovskite (host) lattice was achieved ten inorganic salts [29]. Since MXenes are compact, the guest
upon the preparation under the oxidizing atmospheres, and molecules in MXenes can be easily intercalated. Dimethyl
the nano-sized metallic particles on the surface under reduced sulfoxide, hydrazine, and urea can act as guest molecules.
atmosphere conditions have been prepared by using an in situ For instance, N2H4 (hydrazine), which is analogous to the
growth approach [25]. Chemical vapor deposition (CVD) is basal MXene plane, can be intercalated to form a monolayer
another well-known process where the substrate is subjected into Ti3C2(OH)2. The intercalation strengthens the lattice pa-
to one or more unexpected reactants that react and decay on rameter of MXene c (a parameter of a crystal structure linearly
the surface of the substrate to produce the required thin film correlated to the distance between certain MXene layers) that
deposition [26]. decreases the connection between MX ion layers, and ion
MXenes are usually synthesized by a top-down system- such as Li+, Pb2+, and Al3+can also be intercalated with
atic etching technique as depicted in Fig. 6. This synthesis MXenes [30].
technique is considered a versatile technique because there DMSO can also be used as an intercalation agent, and it is
is no degradation or alteration of the properties of the ma- intercalated into powders of ML-MXene to aggressively ex-
terial when the batch size is increased. The processing of tract the interlayer binding and then followed by the ultra-
MXene through etching the MAX step occurs primarily by sound therapy (Sonication) to obtain the Ti3C2Tx nanosheets
the use of solid etching solutions containing fluoride ions [29, 31, 32], and the process is represented in Fig. 7.
(F−) such as HF, NH4HF2, and a blend of HCl and LiF. For
example, Ti3C2Tx MXene is fabricated by randomly etch-
ing the Ti3AlC2 (MAX) layers by using HF and LiF/HCl 3 Physiochemical properties of various
[27]. Ti4N3 MXene was first identified as the MXene ni- MXenes
tride, and it is synthesized from MXene carbide using a
separation process. To synthesize Ti4N3, the MAX step MXenes are having an excellent electrical and mechanical
Ti4AlN3 is combined with the combination of liquid eutec- properties. The hydrophilic surfaces of the MXenes are ready
tic fluoride salt such as lithium fluoride, sodium fluoride, to bond with different species and show high negative zeta
and potassium fluoride operated at high temperatures. This potential also allowing to form a stable colloidal solution in
process is based on Al, which generates multilayer Ti4N3 water, which makes an effective electromagnetic waves ab-
that could be delaminated further into single and few layers sorption contributes to a huge volume of electromagnetic
by dipping MXene in tetra butyl ammonium hydroxide waves. The various properties of MXene are represented in
followed by sonication process [28]. Fig. 8. However, the electronic and structural reported values

M3AX2 M4AX3
M2AX

Etching “A” layer from Mn+1AXn + Sonication MXene

M 2X
M3X2 M4X3
Fig. 6 Synthesis of MXenes by a top-down selective etching process
emergent mater.

Fig. 7 Preparation of MXenes by intercalation method

are mostly theoretical, and very few experimental publications defined structure. Furthermore, they are theoretically defined
were reported in the ferromagnetism or topological insulators well. MXenes are having a magnificent property because of its
[33]. structure. The carrier mobility of MXene is around ~74100
In general, MXenes without surface termination is sup- and ~22500 cm2 V−1 s−1 along with different directions with a
posed to be magnetic. However, MXenes like Cr2C, Cr2N, bandgap of 0.05 to 2.87 eV in the case of Mo2TiC2(OH)2 and
and Ta3C2 are predicted to be ferromagnetic, and on the other Sc2CO2 MXene. Sc2CF2 MXene with 50 μm flake length is
hand, Ti3C2 and Ti3N2 MXenes are anti-ferromagnetic. having an electrical conductivity of around 9880 S cm-1 and
Monolayers of MXene are forecasted to be metallic material thermal conductivity of 722 Wm -1 K -1 , respectively.
because there is a high electron density at the Fermi level. The Mechanical properties of MXenes are also noticeable with
bandgap of MXene is depending on the surface chemistry of the results; the Young’s modulus (502 GP in-plane) and ten-
MXenes [34–36]. However, the magnetic properties of sile strength are around 8.2 MPa for Ti3C2Tx material. The
the MXenes have yet been experimentally confirmed. optical conductivity lies in the middle of the visible light spec-
Since 2011, 20 different types of MXenes were synthe- trum with 40% of the variation for the Ti3C2Tx MXene. The
sized. Each of them has excellent properties and a well- work function of Nb2CTx MXene is around 4.1 eV [37].

Fig. 8 Excellent properties of MXenes

 emergent mater.

Figure 9 depicts the electrical conductivities of MXenes vacuum-filtered delaminated MXene sheet shows that the me-
before and after annealing conditions. The measured conduc- chanical properties of a single- or two-layer nanosheet have
tivity of Mo2CTx before annealing is approximately around proven to be quite challenging and also with the help of an
0.80 S cm−2, which is increased to 1.2 S cm−2 by the end of the atomic force microscope. The chip elastic properties of bilayer
annealing process. However, the electrical conductivity of and monolayer Ti3C2Tx were analyzed, and it was found to be
Mo2TiC2Tx MXene will enhance twice the magnitude after 0.33 TPa [45]. The various properties of titanium carbide
curing the MXene material at 120°C for 18 h under vacuum MXene (Ti3C2Tx) are shown in Fig. 10.
conditions [38, 39]. The conductivity of pristine Mo2TiC2Tx
and Mo2Ti2C3Tx MXene is measured to be 44 S cm−1 (1494 S
cm−1) and 15 S cm−1 (614 S cm−1), respectively [40]. After the
first annealing cycle, the conductivity of MXene and Seebeck 4 Energy storage application of MXenes
effect will stabilize, in such a case the material Mo2CTx and and MXene-based nanocomposites
Mo2TiC2Tx will act as metal, besides Mo2Ti2C3Tx material
shows a semiconductor property, and it is purely depending MXenes are very good electrical conductors and their surface
on a majorly used MXene (Ti3C2Tx) which is having abun- termination can be easily tunable which plays an important
dant specific capacity due to the prolific pseudo capacitive role in energy storage applications. The synthesis feasibility
sites in it [41]. Upon analysis, the maximum theoretical ca- of MXenes and their stability as colloidal suspensions in water
pacity of Ti3C2Tx material is around ~ 615 C g−1 in −0.6–0 V; along with its various organic solvents render will help in
furthermore, the experimental results also show 135 C g−1 in scaling up of MXene in large quantity. MXenes are highly
0.55 V [42] but is very much lesser than the theoretical capac- known for their hydrophilicity and peek electrical conductiv-
ity. Although N -doped MXenes are fabricated by the ities, and the various properties of MXenes and their applica-
solvothermal process, here nitrogen-doped Ti3C2Tx is synthe- tions are shown in Fig. 11. From the figure, it is observed that
sized and got a high capacitance of around 2836 F cm−3 or 927 MXene will be a promising material for energy storage appli-
F g−1 at 5 mVs−1, in 3M H2SO4 electrolyte, and it created a cations, electromagnetic interference shielding, transparent
benchmark result for all the known MXenes. Also, MXenes conductive electrodes, etc.
are having a relevant electronic band structure. Its metallic Table 1 compares different synthesis approach to obtain
behavior can be turned out by forming additional T-X bonds MXene-based materials used in different energy storage ap-
with the neighboring material. The MXene Sc2C(OH)2 is hav- plication which include LIBs, SC, and hybrid capacitor.
ing a direct bandgap; however, the majority of MXenes have MXene-based LIB shows the capacity of 544 mAh g−1 @
indirect band gaps [43, 44]. 1.75 C rate for the material PVP-Sn(IV)-modified Ti3C2 syn-
The greater electrical conductivity of MXene is due to its thesized using liquid-phase immersion procedure, and also
functionalization of material. If the film thickness is increased, other materials such as Nb2CTx/10%CNT (carbon nanotube)
the optical transmittance is decreased accordingly up to 86 %, sheet and Mo2CTx–CNT sheet have achieved the capacity of
and hence, the sheet resistance is also decreased to a value of around 420 mAh g−1 @ 0.5C and 250 mAh g−1 @ 5 A g−1.
330 Ω sq−1. A single nanosheet (~1.2-nm thickness) leads to a Also, the flexible clay-like Ti3C2 MXene electrode showed
loss in transmittance of ~3%, which is common to that of better performance in SC of 25 m F cm-2 and excellent
graphene nanosheets (~2.3% loss per layer, 0.34 nm). The cyclability of 10000 cycles. Apart from lithium storage,
sodium-ion batteries are studied more, where 2D MXene

(a) (b)
2410
T
x

850
T
x

C
2
C
2

Ti
2
Ti
2

614
Tx
Tx

15
)C
2
)C
2

Ti
2
Ti
2

o
2
o

(M
2
(M

Tx

1494
Tx

44
)C
2
)C
2

Ti
Ti

o
2
(M
o
2
(M

0.8 1.2 After Annealing

Tx

Before Annealing
Tx

C
C

o
2
M
o
2
M

0 10 20 30 40750 780 810 840 870 0.0 0.4 0.8 1.2 1.6 700 1400 2100 2800
Electrical conductivites (S.cm-1) Electrical conductivites (S.cm-1)
Fig. 9 Electrical conductivities of MXenes before annealing and after annealing
emergent mater.

Vis-NIR Plasmon Ion Electrically

Resonance Storage Conductive

1000 S cm-1
Visible
Ion Storage Transparency
1500 F cm-3 97% T/nm

Hydrophilic 0.33 TPa

Mechanical
surface strength
Biocompatibility

Fig. 10 Properties of titanium carbide MXene (Ti3C2Tx)

electrodes are evaluated more. Filtration synthesis of porous interesting material of SC due to their interesting characteristic
Ti3C2Tx/CNT and Mo2CTx-CNT paper delivers the anode property. The high specific surface area with nanosized pores
capacity of 345 mAh cm−3 and 700 F cm−3 (196 F g−1) in a and open channels are very important features for high-
sodium-ion battery system. performance SCs. For example, Ti3C2 MXene-based SC elec-
trodes in aqueous solutions showed excellent cyclic ability
4.1 MXenes as supercapacitor electrodes and volumetric capacitance of 300–400 F cm−3, which shows
three times higher than activated carbon and graphene-based
ECs usually have higher power densities than LIBs. capacitors. Ti3C2 MXene clay has a volumetric capacitance of
Nevertheless, energy densities are considerably less. It has a 900 F cm−3, a higher capacity per unit volume than other
higher energy density but low power density in the battery materials. FL-Ti3C2 nanolayers can be tightly mixed with
systems. Similarly, to increase voltage and conductivity while polyvinyl alcohol (PVA) polymers, forming MXene-PVA
preserving stability, advances in electrolytes are required [55]. layered structures. The electrical conductivity of the compos-
It is of utmost importance to know how materials are treated ite material can be controlled from 4×10−4 to 220 S cm−1 (by
and transferred via electrode-electrolyte interfaces and will varying the MXene content from 40 to 90%). The composites
have good knowledge of the processes of charge transfer. have a strength of up to 400% higher than flat MXene films
The ability to synthesize compact, high surface area nano- and have an increased value of 500 F cm−3. The substitute
structured electrodes offers the ability to store various charges filtration process for the formulation of MXene-carbon
at a single site, improving the rate of charge. nanomaterial composite film is also being invented. In SC,
More surface features can also provide a reproducible and these composites showed improved performance at high rates.
powerful capacity for energy storage and fast charge and dis- The addition of polymers/carbon nanostructures between
charge. The design of new materials with special structures some of the layers of MXene allows it simpler for the electro-
designed to withstand capacitive loads efficiently will be lyte ions to diffuse through the MXenes, the secret to their use
spurred with advanced methodologies (computational and an- in versatile SCs. The high conductivity of composite is
alytical) for the production of the material. These methods will highlighted by electrochemical measurements, which is likely
also have the molecular insight needed to evaluate the physi- due to the small insulation gaps between the MXene flakes
cal and chemical requirements of the electrolytes with higher and the thin CNFs; vacuum pressing also does not significant-
voltages, improved ion conductivity, and great electrochemi- ly reduce the capacitance of the MXene flakes. Cyclic stability
cal and thermal stability. In this concern, MXenes have been revealed 100% retention of capacity after 10,000 cycles [56].
 emergent mater.

Lithium Ion
Battery

Sodium Ion
Battery

Supercapacitor

Lithium sulfur
Battery
Lithium Ion
Capacitor

Fig. 11 MXenes and MXene-based nanocomposites as electrical energy storage materials

Figure 12 shows the schematic diagram of the MXene SC. and bridges the gap between the two systems. Figure 13 rep-
Free-standing Ti3C2Tx MXene/carbon nanofiber electrodes are resents the MXene-based hybrid capacitor. Lithium-ion ca-
widely used. It is prepared by electrospinning technique, Firstly, pacitor (LIC) is one of the well-known conventional hybrid
Ti3C2Tx MXene flakes were dispersed in PAN solution. Then capacitors.
the solution is coated onto the substrate mat followed by carbon- MXenes are becoming a promising material for flexible
izing the fiber networks under an inert atmosphere. The carbon- LIC devices. To date, numerous electrode materials were used
ized fiber mat is free standing and free from a binder and additive in LIC systems. Owing to the various Li-ion storage struc-
compounds. Hence, it can act as an self standing electrode for the tures, anode materials for LICs are classified into three groups
SC and the addition of composite material to the MXene elec- as insertion, conversion, and alloy type and depicted in Fig.
trode shows stable and durable performance [57]. So, N2-doped 14. The insertion type materials, such as graphite, hard carbon,
2D (N-Ti3C2Tx) MXene material was found to be a better SC. It TiO2, Li4Ti5O12 (LTO), and Nb2O5, have a stable structure.
was fabricated by post-etch annealing Ti3C2Tx in ammonia so- However, their lower theoretical capacity (< 400 mAh g–1) or
lution to obtain N-Ti3C2Tx [58]. high-voltage plateau vs. Li metal made the insertion type ma-
terial inhibits in maximum use. Second, the alloy-type (Si, Sn,
4.2 MXenes based hybrid capacitors and Sn-based composites) and conversion-type (MoS 2,
MnO2, Fe3O4, CoO) materials have a high theoretical capacity
The hybrid capacitor is a type of energy device which com- (>700 mAh g–1) than insertion type material. However, the
bines the properties of both SC and LIBs in a single system strong irreversible strength, large volume change, and slow
emergent mater.

Table 1 Comparison of different MXene-based electrodes with their synthesis methodology in various energy storage applications

Materials Etchant Synthesis approach Capacity of anode Current density Retention No. Ref.
(mAhg−1) (Ag−1) (%) cycles

Li-ion battery Nb2CTx/10%CNT paper Filtration 420 0.5 C 100 100 [44]
Mo2CTx – CNT paper Filtration 250, 75 5 Ag−1 - 10,000 [46]
10 mAg−1
PVP-Sn(IV)-modified Liquid-Phase immersion 544.0 0.5 94.30 200 [47]
Ti3C2 procedure (1.75C)
Nb4C3Tx/Nb2O5 CO2 oxidation by one-step 208.0 50 mAg−1 (0.25 C) 94 400 [48]
NIB Porous Ti3C2Tx/CNT Filtration 345 mAh cm−3 0.1 100 500 [44]
Mo2CTx-CNT paper Filtration 700 F cm−3 10 100 10,000 [46]
LIC CTAB-Sn(IV)@Ti3C2 Filtration 33 F g−1 2 71.70 4000 [49]
Nb2O5/Nb2CTx One-step CO2 oxidation 600 m F cm−2 - - 400 [50]
Hybrid Cathode: LiFePO4 - 50–70 Wh L−1 - - - [51]
capacitor Anode: Nb2CTx/CNT
Cathode: - 160 Wh kg−1 @ 220 W - - - [52]
LiNi1/3Co1/3Mn1/3O2 kg−1
Anode: Ti2CTx
Supercapacitor Clay-like Ti3C2 MXene Filtration 25 mF cm−2 2 mAcm-2 92 10,000 [53]
PPy/Ti3C2Txfilm Filtration 1000 Fcm−3 5mVs−1 92 25,000 [54]

kinetics of such materials cause severe electrode polarization durability of the ring. From this point of view, materials with
and decay over cycling. The key problems for the anode are a well-designed or nano-sized design can effectively minimize
the development of electronic/ion conductivity and the the Li+ diffusion path and improve the transport of electrons.

Fig. 12 Schematic representation of MXenes-based supercapacitor electrodes and their electrochemical energy storage mechanism
 emergent mater.

Fig. 13 The principal mechanism

of MXene-based hybrid capacitor

The most widely used cathode materials for LIC are demonstrate non-ideal battery behavior but are close to a ca-
graphene, AC, and CNTs. Among different materials, AC pacitor that suggests their use in LICs [59, 60]. Moreover, the
has gained much attention due to its specific surface area, ease properties of energy recovery, the stability of MXenes, and the
of synthesis, nontoxicity, and less cost. However, its narrow electronic transmission speed are greatly influenced by func-
pore size distribution and pore channels inhibit the diffusion tional groups (−O, −Cl, −F, −OH,) on the surface of MXene
of the electrolyte ion, and comparatively low electron conduc- layers.
tivity results in a low power density. As a result, materials with Table 2 shows that the various MXene electrodes were
a wide surface area and an acceptable pore size distribution synthesized by different approaches and etchant to obtain a
can effectively increase the flexibility and power efficiency of high-capacity electrode for hybrid LIC application. From the
LICs. As a full-cell hybrid electrochemical capacitor, the LIC table, it is observed that compared to single MXene material
requires a large-capacity Li+ reversible intercalation anode to (Ti 3 C 2 T x and Ti 2 CT x ), composite flexible material
achieve advanced electrochemical energy recovery. MXenes (Ti3C2Tx@Fe2O3 and CTAB-Sn(IV)@Ti3C2) showed high
like Ti3C2Tx, Ti2CTx, Nb2CTx, and V2CTx have a unique, specific capacity. For example, Ti3C2Tx and Ti2CTx elec-
extremely thin, fully accessible layer structure that eases the trodes showed an anodic performance of 226 F cm−3 @ 10
intercalation/deintercalation kinetics of Li+. Thus, MXenes mVs−1 and 250 mAhg−1 @ 20 mAg−1 with a corresponding

Fig. 14 Various anode materials for Hybrid capacitor

emergent mater.

Ref.

[49]

[61]
[52]

[45]

[62]

[52]
20.7μWhcm−2 2.2 mWcm−2 [63]
energy density of around 20.7μ Wh cm−2 and 160 Whkg−1.
On the other hand, the composite MXene Ti3C2Tx@Fe2O3
P (W kg−1) and CTAB-Sn(IV)@Ti3C2 electrode showed the maximum
anodic capacity of 1180 mAhg-−1 @ 0.1Ag−1 and 675
400

495
258

220
mAhg−1 @ 0.1 Ag−1 which contributes to the high energy

50-70 WhL−1 -
density value of 216 Whkg−1 and 105.6 Wh kg−1 for the
Capacity of anode (mAhg−1) Current density (Ag−1) Voltage (V) E (Wh kg−1)

325 Fcm−3
composite system.

105.6
216

160
67
5 MXene-based hybrid supercapacitors
0.4–4.2
0.01–4

as next-generation energy storage device

1–4
1–4

0–3

0–3
0–2
for flexible electronics applications

The innovation of wearable energy storage devices was

motivated by the increasing need for wearable electron-
ics. MXenes are regarded as promising flexible elec-
50 mA g-1

50 mAg−1
10 mVs−1

trodes owing to their high conductivity, ultra-high volu-

0.5C
0.02

metric capacitance, excellent hydrophilic properties, and

0.1

0.1

surface action. In order to help researchers in MXene

research, different mechanical, electrical characteristics
are correlated for the production of high-quality portable
energy storage systems at the core of the design of wear-
able consumer electronics [54]. Advances in electrodes
1180 mAhg−1

489 mAh g−1

270 mAh g−1

400 mAhg−1

226 F cm−3

and electrolytes have given a strong solution to the trade-

off between energy and power densities. However, these
675

250

traditional energy storage systems are usually operation-

ally rigid or non-mobile, limiting their use in flexible
Amine assisted delamination and filtration

electronics. To solve this problem, the development of

flexible electrodes with excellent durability and strong
TBAOH delamination and filtration

TBAOH delamination and filtration

electrochemical efficiency is necessary to meet the criti-

cal requirements of portable energy storage systems.
MXenes, a new class of 2D materials generated by “A”
Liquid-phase immersion

layer insulation from the MAX phases, have gained sig-

Synthesis approach

nificant interest in the field of flexible energy storage

LiF/HCl etching
MXene-based electrodes for hybrid lithium-ion capacitors

technologies.
9M HCL+7.5M LiF, Surfactant

The advantages from outstanding properties such as

LiF/HCl
Etching

lateral microscale, atomic layer thickness, and exceptional

hydrophilic properties enable MXenes to be easily
mounted into flexible film/sheet electrodes using simple
+5M LiF, 9M HCL
50% HF, 6M HCl

9M HCl+1.9M LiF,
Delaminated Ti3C2Tx/CNT 9M HCl+3.8M LiF,

Precursor- Nb2AlC
12M HCl+3M LiF

vacuum filtration or spray technology. In contrast,

+ 49% HF, 6M

Precursor-Ti2AlC

MXenes have demonstrated a considerably volumetric ca-

HCl+LiF

pacitance than conventional carbon-based materials, ren-

10% HF

50% HF
Etchant

dering MXenes superior to lightweight, compact electron-

ics. Also, the excellent conductivity of MXenes leads to
Delaminated Nb2CTx/CNT -
-

an exceptionally higher power density than the metal ox-

ides of the semiconductor form, which leads to the fulfill-
CTAB-Sn(IV)@Ti3C2

ment of the need for the fast-charging functionality of

recent consumer electronics. The surface chemistry com-
Ti3C2Tx@Fe2O3

Nb2CTx/CNT

bined with the high electro-negativity of MXenes will

result in the etching of HF acid also makes it possible to
Materials

Ti3C2Tx
Table 2

Ti2CTx

fuse MXenes with other nanomaterials to prepare high-

performance versatile composite electrodes.
 emergent mater.

Fig. 15 Flexible MXenes-based supercapacitor

5.1 Fabrication of flexible electronics (role to role such as NH3 and CH3COCH3. In addition to detecting gases,
fabrication) MXenes can track minor alterations in stress and strain due to
the transmitted layer composition and splendid mechanical
The attractive physical, chemical, and biological characteristic properties of the MAX phases. For example, pure Ti3C2Tx
and properties of MXene finds a wide utility and also utilized MXene film possesses high versatility, so it finds an applica-
in the application of biosensors, nanogenerators, and electro- tion in highly sensitive piezoresistive sensors [64]. The sensor
magnetic interference shielding (EMI) fields. However, 2D system operates with the sensing and measuring the value
MXenes incorporates many characteristics, such as layered with the external forces which are attributed to the significant-
composition, metallic conductivity, surface chemistry, and ly improved interlayer spacing of MXene. This effort and
hydrophilicity, which are of huge importance for sensor appli- advantage offered by MXenes find an application in mechan-
cations. In particular, the biocompatible, non-toxic, and de- ical sensors [65]. Also, a versatile strain sensor based on the
gradable properties of MXenes are critical for bio- and gas flexible Ti3C2Tx MXene/CNT film was also prepared by layer
sensors applications. Due to the extraordinary characteristics, assembly of the air spray coating process.
MXenes have superior qualities to other extensively reported Later, a mixture of MXene and PVA hydrogel was devel-
2D materials such as graphene and MoS2. For example, gas oped to demonstrate a high conductive and sensitive strain
such as NO2− and H2O2 is detected by using Nafion/Hb/ sensor with outstanding stretchability, for an instant, self-
MXene Ti3C2Tx/Glassy carbon electrode (GCE). MXene- healing capacity, excellent conformability, and adhesiveness
based flexible Ti3C2Tx/graphene oxide (GO) electrodes were to satisfy the complex specifications of wearable electronic
fabricated by using inkjet printing technology which exhibited devices. These activities show a significant versatility of
an outstanding performance for H2O2 detection. MXenes in compact sensor systems for environmental mea-
Furthermore, MXenes are capable of detecting brominated surement and stress detection. In addition, the characteristics
(BrO3−) compounds and volatile organic compounds (VOCs), of high conductivity and electronegative surface derived from
emergent mater.

Fig. 16 Potential and versatile applications of MXenes in various fields

negatively charged functional groups also classify metallic Fe(OH)3 nanoparticles with a pore diameter of 3–5 nm. In this
MXene as a popular candidate for nanogenerator applications. process, the nanoparticle is placed into the MXene film by
For example, Ti3C2Tx MXene was successfully synthe- dissolving the Fe(OH)3 nanoparticles than accomplished by
sized and demonstrated as a self-charging power unit carrying outing low calcination temperature at 200°C, which
consisting of a compact triboelectric nanogenerator and mi- leads to the formation of highly linked nanopore channels that
cro-SCs. Dong et al. have created a versatile nanogenerator facilitate effective ion transport without sacrificing ultra-high
based on Ti3C2Tx MXene to capture the low power generated density. As a consequence, the altered nanoporous MXene
by human muscles. Also, the merits of metallic conductivity, film poses an attractive volumetric capacitance (1142 F cm−3
active chemical surfaces, and excellent hydrophilicity make it at 0.5 A g−1) and good rate capability (828 F cm−3 at 20 A
possible for MXenes to play a significant role in the EMI g−1). But still, the material is possessing a high volumetric
shielding region. Furthermore, Han et al. has also recorded capacitance of 749 F cm−3 even at a higher active mass load-
the excellent EMI performance for the Ti3C2Tx MXene and ing of 11.2 mg cm−2. Therefore, this flexible and free-standing
reported a value of about 76 dB with a thickness of 1 mm. nanoporous MXene film is a promising electrode material for
Later, Shazard et al. has also developed a series of flexible and flexible, portable, and compact storage devices [66]. The var-
ultra-thin MXene films based on Ti3C2Tx, Mo2TiC2Tx, and ious application of MXene-based flexible SC is presented in
Mo2Ti2C3Tx flakes materials and recorded exemplary EMI Fig. 15.
performance.
5.3 Applications of MXenes
5.2 Flexible supercapacitors
MXenes are having different structural characteristics, and
MXene films find a desirable application in SC electrodes due their versatile nature made them promising material for sever-
to their ultra-high-power density and pseudocapacitive charge al potential applications. Among the potential applications,
storage mechanism. However, the self-discharge of MXene the energy storage and conversion of MXenes were initially
nanosheets has a significant influence on their capacity rate identified and extensively reported by several research groups.
and energy storage. A self-contained and versatile altered However, numerous other applications of MXenes are ex-
nanoporous MXene film is manufactured by inserting plored in recent years and represented in Fig. 16. For instant,
 emergent mater.

freestanding Ti3C2Tx MXene film exhibits the highest elec- an extensive investigation is required to further demonstrate
tromagnetic interference shielding ever reported for a synthet- these materials for realistic applications.
ic material of comparable thickness. Apart from the energy
storage application, MXenes find application in other fields,
such as biosensors, flexible electronics, nanogenerators, ener- Acknowledgements The authors greatly acknowledge the funding sup-
port from the technical research center (TRC) project (Ref. No. AI/1/65/
gy harvester, thermoelectric, inkjet printing, photocatalyst, lu-
ARCI/2014 (c)) sponsored by the Department of Science and Technology
bricants, water purifications, reinforcement for composites, (DST), Government of India, New Delhi, India.
and photothermal therapy, which have reported by other re-
search groups [67–74].
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