Friction 12(1): 39–51 (2024) ISSN 2223-7690

https://doi.org/10.1007/s40544-022-0726-2 CN 10-1237/TH
RESEARCH ARTICLE

Achieving near-infrared-light-mediated switchable friction

regulation on MXene-based double network hydrogels
Pengxi WU1, Cheng ZENG1, Jinglun GUO1, Guoqiang LIU1,*, Feng ZHOU1,2,*, Weimin LIU1,2
1
Center of Advanced Lubrication and Sealing Materials, State Key Laboratory of Solidification Processing, Northwestern Polytechnical
University, Xi’an 710072, China
2
State Key Laboratory of Solid Lubrication, Lanzhou Institute of Chemical Physics, Chinese Academy of Sciences, Lanzhou 730000,
China
Received: 29 June 2022 / Revised: 13 October 2022 / Accepted: 21 November 2022
© The author(s) 2022.

Abstract: MXene possesses great potential in enriching the functionalities of hydrogels due to its unique
metallic conductivity, high aspect ratio, near-infrared light (NIR light) responsiveness, and wide tunability,
however, the poor compatibility of MXene with hydrogels limits further applications. In this work, we report a
uniformly dispersed MXene-functionalized poly-N-isopropylacrylamide (PNIPAM)/poly-2-acrylamido-2-methyl-
1-propanesulfonic acid (PAMPS) double network hydrogel (M–DN hydrogel) that can achieve switchable
friction regulation by using the NIR light. The dispersity of MXene in hydrogels was significantly improved by
incorporating the chitosan (CS) polymer. This M–DN hydrogel showed much low coefficient of friction (COF)
at 25 °C due to the presence of hydration layer on hydrogel surface. After illuminating with the NIR light, M–DN
hydrogel with good photothermal effect rapidly raised the temperature to above the lower critical solution
temperature (LCST), which led to an obvious increase of surface COF owing to the destruction of the hydration
layer. In addition, M–DN friction control hydrogel showed good recyclability and controllability by tuning
“on-off” of the NIR light. This work highlights the construction of functional MXene hydrogels for intelligent
lubrication, which provides insight for interface sensing, controlled transmission, and flexible robotic arms.

Keywords: MXene dispersion; photothermal hydrogel; near-infrared (NIR) light; friction modulation

1 Introduction stimulation, active regulation is more controllable.

In modern society, with increasing environmental
complexity, the research and development of artificial
intelligence materials is on the agenda. Stimuli-
responsive interface materials can rapidly achieve
reversible physical or chemical property transformations
when stimulated by temperature, pH value, magnetic
field, light, and so on [1–5]. These materials are
mainly based on stimuli-responsive polymers [1]
and phase-change materials [6]. On the basis of the
original response, adding nanoparticles to enrich the
versatility of materials has become the main research
direction [1, 7, 8]. Meanwhile, compared with passive
Poly-N-isopropylacrylamide (PNIPAM)-based
hydrogels have become representative stimuli-
responsive hydrogels. When below the lower critical
solution temperature (LCST), the PNIPAM molecular
chain stretches. Hydrogen bonds are formed, which
causes the appearance of a hydrated layer. In contrast,
when above the LCST, the PNIPAM molecular chain
shrinks. The hydrogen bonds are broken, which
causes the disappearance of the hydrated layer [9].
Taking advantage of this property, it has been widely
used in many situations, such as drug delivery [10],
temperature sensors [11], smart actuators [12], friction
regulation [13–15], and so on. Among them, the

* Corresponding authors: Guoqiang LIU, E-mail: guoqiangliu@nwpu.edu.cn; Feng ZHOU, E-mail: zhouf@licp.cas.cn
40
application of friction regulation has gradually
attracted attention. For example, Zhu et al. [16]
combined PNIPAM as a coating on the surface of
polydimethylsiloxane (PDMS) to achieve mutual
conversion between hydrophilic lubrication and
antibacterial properties. To achieve active regulation,
incorporating materials that respond to stimuli-
responsive heating inside PNIPAM hydrogels becomes
particularly important. Chen et al. [13] fixed Fe3O4
inside PNIPAM microgels and realized the purpose of
actively utilizing the stimulus response of near-infrared
(NIR) light to control the COF of water lubrication.
MXene is a kind of two-dimensional lamellar
material composed of transition metal carbides, nitrides,
or carbonitrides with unique metallic conductivity,
high aspect ratio, near-infrared photoresponsivity, and
widely tunable properties [17]. In addition, Ti3C2Tx is
one of the most widely used MXene materials, where
Tx represents different surface termination groups
(e.g., OH, O, and F) [17–19]. Because of its excellent
properties, MXene is widely used to realize the
functionalization of hydrogels. For example, the
excellent electrical conductivity and two-dimensional
sheet structure is conducive to the preparation
of motion sensors, electrical conductivity and NIR
light stimuli-responsiveness benefit the preparation
of programmable stimuli-responsive hydrogels and
the electromagnetic shielding ability helps prepare
electromagnetic shielding materials [12, 20, 21].
However, the applications of MXenes for switchable
friction regulation are deficient. In previous reports,
MXene easily exhibits agglomeration behavior. This
is because various interactions between the MXene
surface groups and the polarized groups of various
molecules can form in the hydrogel prepolymerization
solution [22, 23]. It is particularly important to make
MXene disperse uniformly in the hydrogel, which
can increase the utilization of MXene and prevent the
hydrogel from bending due to uneven distribution.
In this work, we utilized hydrogen bonding between
CS and MXene nanosheets, which greatly reduced
the possibility of contact between the surface groups
of MXene nanosheets and various molecules in the
prepolymerization solution. Moreover, the larger
viscosity of the CS solution slowed the settling rate
of the inner nanosheets. The treated CS–MXene was
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Friction 12(1): 39–51 (2024)
then combined with the traditional double-network
hydrogel [24], in which 2-acrylamido-2-methyl-1-
propanesulfonic acid (AMPS) was used as the first-layer
network and NIPAM was used as the second-layer
network. M–DN hydrogels that can realize the
regulation of the COF at the interface by NIR light
were prepared. The large amount of free-flowing water
inside the M–DN hydrogel provides the possibility
for hydration lubrication. During the friction process,
the free-flowing water was affected by the amide
groups on PNIPAM and formed a hydrated layer,
which can reduce the COF between the interfaces.
When irradiated with NIR light, the MXene nanosheets
reacted rapidly and generated a large amount of heat.
As the temperature increased, PNIPAM underwent
a phase transition. The hydrogen bonds between
PNIPAM chains and water molecules were broken.
Thus, the hydrated layer was destroyed, and the COF
was increased on the interface [25–27].
Through this work, MXene (Ti3C2Tx) nanosheets
were treated through hydrogen bonding interactions
between CS and MXene, which caused MXene to
be coated with chitosan to weaken the interaction
between AMPS and MXene. In this way, a dispersion
method of MXene nanosheets in hydrogels was
proposed. Thus, the friction regulation of the hydrogel
surface through the photothermal effect of MXene
nanosheets was realized, which further expanded the
application of MXene hydrogels. This friction-tunable
hydrogel has great potential in the fields of friction-
interface sensing, intelligent manipulators, and
controlled transportation.
2 Experimental
2.1 Preparation of MXene nanosheets
MXene nanosheets were prepared in two main steps.
First, Ti3AlC2 (MAX) was etched to obtain few-layered
Ti3C2Tx MXene flakes. 3.2 g of LiF, 10 mL of pure water,
and 30 mL of concentrated hydrochloric acid were
added to a 50 mL polytetrafluoroethylene beaker.
The mixed solution was placed in a water bath with a
stirrer at 40 °C. Subsequently, added 2 g of MAX into
the beaker in several portions. The reaction lasted for
24 h. Then, the solution was centrifuged many times
Friction 12(1): 39–51 (2024)
(3,500 rpm, 5 min) using pure water until the liquid
in the centrifuge tube was no longer translucent. The
suspension containing few-layered MXene flakes was
collected. The collected suspension was centrifuged
(10,000 rpm, 10 min) to remove water. Thus, few-layered
MXene flakes could be obtained after the freeze-
drying treatment of the sedimentation. Second, 200 mg
of freeze-dried MXene was added to a 100 mL
jacketed reactor with 50 mL of pure water. The above
dispersion was sonicated for 2 h at 10 °C with 30%
power using a probe sonicator. The treated solution was
directly lyophilized to obtain dry MXene nanosheets.
2.2 Preparation of homogeneously dispersed M–SN
hydrogels
2 mg (4, 6, and 8 mg) of freeze-dried MXene
nanosheets was dispersed into 5 mL of pure water
through water bath ultrasonic. Then, added 0.1 g of
CS into the solution. Two drops of glacial acetic acid
were added to help dissolve the CS. The above solution
was stirred at high speed for 1 h. The subsequent
solution was labelled as solution A. Next, 4 g of
2-acrylamido-2-methylpropanesulfonic acid (AMPS),
90 mg of MBAA crosslinker and 10 mg of 2-oxoglutaric
acid initiator were added to 5 mL of pure water to
obtain homogeneous solution B. Solutions A and B
were uniformly mixed, and the air bubbles in the
mixed solution were removed through water bath
ultrasonic. Then the mixture was photoinitiated
under UV irradiation for 30 min to form a covalent
cross-linked hydrogel with MXene intercalation.
Finally, the prepared hydrogel was immersed in pure
water for 24 h to obtain the M–SN hydrogel.
2.3 Preparation of homogeneously dispersed M–DN
hydrogels
4 g of NIPAM, 5.4 mg of MBAA crosslinker, and
10 mg of 2-oxoglutaric acid initiator were added to
20 mL of pure water to obtain a homogeneous
PNIPAM prepolymerization solution. Then, the M–SN
hydrogel was placed in a petri dish to fully soak
in the prepolymerization solution at 20 °C for 48 h.
The treated SN hydrogels were removed. The upper
and lower surfaces of the hydrogels were adequately
covered by glass plates. Double network hydrogels
with uniformly dispersed MXene were obtained by UV
41
light initiation at 20 °C for 30 min. Finally, the M–DN
hydrogels were immersed in pure water for 24 h.
2.4 Characterization
An X-ray diffractometer (Bruker D8 X-ray, Germany)
was used for X-ray diffraction (XRD) measurements.
Transmission electron microscopy (TEM) (FEI, Talos
F200X, and USA) was used to characterize the
morphology of MXene nanosheets. Porous morphology
of lyophilised hydrogel sections obtained by scanning
electron microscopy (SEM) (FEI, Helios G4 CX).
Characterization of CS and MXene interactions was
performed using a TENSOR II Fourier transform
infrared (FTIR) spectrometer (Bruker, Germany). The
size of the MXene nanosheets was measured using
a particle size analyser (Malvern Instruments, UK).
X-ray photoelectron spectroscopy (XPS) (PHI 5000
VersaProbe III) with an Al Kα X-ray source was
used for elemental analysis. For the photothermal
performance study, M–DN hydrogels were placed in
a petri dish with appropriate pure water. Then, they
were irradiated with an NIR laser (BST808-5-F, Xi'an
Best Laser Optronics Co., Ltd.) at a wavelength of
808 nm. The irradiation diameter and distance were
1 mm and 5 cm, respectively. The temperature was
measured by infrared thermography (FLIR, E8-XT,
and USA).
2.5 Mechanical performance tests
The tensile strength at break of the M–SN hydrogel
and M–DN hydrogel was tested using a universal
mechanical testing machine (INSTRON 5982). For the
test at 50 °C, a layer of silicone oil was applied to
the surface of the hydrogel to prevent water loss. The
constant temperature of 50 °C in the chamber was
remained for 5 min before the test of tensile strength
at break. The sample was processed into I-beam
shape. Their width and length were 4 and 10 mm,
respectively. The stretching speed was 50 mm/min.
2.6 Rheology testing
The G' and G'' moduli of the M–SN hydrogels and
M–DN hydrogels were tested with frequency and
temperature as variables using a rotational rheometer
(HAAKE MARS III, USA). Tests were carried out on
circular hydrogels with a diameter of 25 mm. Frequency
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change tests were carried out from an angular
frequency of 100 rad/s to an angular frequency of
0.1 rad/s. Before the test, the sample was kept at a
constant temperature of 25 °C for 5 min before being
heated to 50 °C at a rate of 2.0 °C/min. The load was
maintained at 0.1 N and the angular frequency at
10 rad/s.
2.7 Tribological test
The tribological properties of the M–DN hydrogels
were tested using a ball–disk contact reciprocating
friction tester (UMT-3, Bruker, Germany). In all tests,
the lower surface was wiped to dry and fixed in the
sink using double-sided tape to prevent slippage
when rubbing. After fixing the M–DN hydrogel in
the water bath, the entire surface of the sample was
kept flat. Deionized water was added to make water
surface parallel to the upper surface of the sample.
An amount of water was dripped between the upper
friction pair and the sample to maintain the hydrated
layer during the whole friction when the NIR light
was switched off. The upper friction pair was made
of glass ball with 5 mm in diameter to maximize the
transmission of NIR light. The reciprocation stroke
was 5.0 mm. The COF was derived with the help
of software by dividing the frictional force by the
normal load.
3 Results and discussion
3.1 Synthesis and characterization of M–DN
hydrogels
Figure 1 shows the dispersion principle of MXene
(Ti3C2Tx) and the preparation process of the M–DN
hydrogel. There were a large number of groups (such
as –OH, –O, and –F) on the surface of the MXene
sheet, as shown in Fig. 1(a). These groups can form
strong hydrogen bonds with the molecular chains
in the hydrogel network. The MXene surface groups
interact easily with the polar groups of various
molecules in the hydrogel prepolymerization solution
[22, 23], which results in the agglomeration of MXene
sheets and prevents the MXene sheet from being

Fig. 1 Dispersion of MXene improvement and the preparation of M–DN hydrogels. (a) Chemical structure of MXene nanosheets;
(b) schematic diagram of the hydrogen bonding interaction between CS and MXene nanosheets; (c) schematic diagram of the preparation of
M–DN hydrogels; (d) comparing dispersibility of MXene before and after improvement; and (e) difference between the CS–MXene@PAMPS
single network hydrogel (M–SN hydrogel) and MXene@PAMPS hydrogel.

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Friction 12(1): 39–51 (2024)
uniformly dispersed in the hydrogel. In addition, this
phenomenon was more apparent as the concentration
of MXene sheets increased. To solve this problem, a
small amount of CS was introduced to promote the
dispersion of MXene, as shown in Fig. 1(b). CS played
a dual role in the MXene dispersion problem. First,
the strong hydrogen bonds between the hydroxyl as
well as amino groups of CS and the hydroxyl groups
on the MXene surface can weaken the interaction
between the MXene surface groups and molecules of
the prepolymerization solution. Second, CS triggered
the transformation of the solution into a sol state
because of its feature of a short-chain polymer, which
could slow down the sedimentation rate of MXene.
On this basis, a method for friction-controlled
M–DN hydrogels was devised [24], which is shown
in Fig. 1(c). The mass of this hydrogel before and
after lyophilization changed from 0.3251 to 0.0512 g,
possessing a water content of up to 84.3 wt%. As
shown in Fig. 1(d), suitable initiators were tested to
verify the effect of CS on the MXene dispersion. The
thermal initiator (potassium persulfate, KPS) and the
photoinitiator (2-oxoglutaric acid) were added to the
same concentration of MXene nanosheet dispersion.
The results showed that KPS caused the agglomeration
of MXene nanosheets quickly, while 2-oxoglutaric
acid did not. Therefore, it was more suitable to use
photoinitiator to prepare hydrogels. In addition, the
monomer also had an effect on the MXene nanosheets.
As shown in Fig. S1(a) in the Electronic Supplementary
Material (ESM), the surface in the etched Ti3C2Tx
contained a large number of hydroxyl groups that
could interact with water molecules, resulting in
excellent dispersion. However, agglomeration rapidly
occurred after a certain amount of AMPS was dissolved.
This was attributed to the phase separation caused by
the interaction between ionized AMPS and MXene.
It was interesting to note that the solution in which
the MXene nanosheets and AMPS were comingled
gradually gelled with time (Fig. S1(b) in the ESM).
This was enhanced with increasing concentrations
of MXene nanosheets. The phenomenon also poses
difficulties for the preparation of MXene hydrogels.
The modification of MXene with chitosan significantly
addressed these problems. When equal concentrations
of MXene and CS–MXene were added to the AMPS
prepolymerization solution, the unmodified MXene
43
agglomerated in 10 s, while CS–MXene still had good
dispersibility after 24 h. The two solutions were
further initiated to form a hydrogel. As shown in
Fig. 1(e), CS–MXene was dispersed uniformly, and the
whole material was not bent. This highly dispersed
method was beneficial to M–DN hydrogels with a
larger receptive specific surface area when irradiated
by NIR light, and the high transparency could promote
fully exothermic irradiation parts.
To uniformly disperse MXene inside the hydrogel,
further reduction of MXene size was considered based
on the previously reported Ti3AlC2 (MAX) etching
method [17, 18]. Probe sonicator was used to obtain
smaller MXene nanosheets (Fig. S2 in the ESM). The
XRD was performed to compare MAX with MXene.
aluminium (Al) was etched completely, and the (002)
peak in the MAX phase was shifted from 9.5° to 7.0°.
Compared with the previously reported multilayer
MXene sheet (002) peak shifts (9.5° to 9.0°), the shift
amplitude of the MAX phase is larger due to the
greater distance between the layers of the sheet [18].
It indicates that few-layer or single-layer MXene
nanosheets were obtained (Fig. 2(a)). The morphology
of MXene nanosheets was characterized by TEM.
It was observed that the MXene nanosheets exhibited
a nanoscale oligomeric state, which was consistent
with the particle size scale tested in Fig. 2(b). Energy
dispersive spectrometry (EDS) analysis showed that
a large number of oxygen (O) and fluorine (F) groups
were distributed on the MXene nanosheet surface,
which demonstrated that the probe sonication
approach did not destroy the various groups on the
MXene surface (Fig. S3 in the ESM). The composition
and changes in the elements of MXene were
investigated by X-ray photoelectron spectroscopy
(XPS). The full spectrum showed distinct peaks of
O and F on the surface of the MXene nanosheets. The
high-resolution XPS spectra of Ti 2p, fitted by Ti 2p3/2
to Ti 2p1/2, were consistent with other previous reports
[28, 29], which confirmed that MXene nanosheets were
successfully prepared (Figs. 2(c) and 2(d)).
After modification by CS, the elements on the
CS–MXene surface were analysed by XPS. It was
evident that the peaks of titanium (Ti) and F did
not appear in the full spectra. Instead, the nitrogen
(N) peak of CS appeared, indicating that CS was
encapsulated on the MXene surface (Fig. 2(c)). The
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Fig. 2 MXene preparation and processing characterization. (a) XRD patterns of MAX and MXene nanosheets; (b) particle size
characterization of MXene nanosheets; (c) XPS full spectra of MXene nanosheets and CS–MXene; (d) Ti 2p XPS spectra of MXene
nanosheets; (e) FTIR spectra of MXene nanosheets, PAMPS@CS hydrogels, and PAMPS@CS-MXene hydrogels; (f) optical pictures of
MXene nanosheets and CS–MXene after freeze-drying; and (g) SEM images: (i) M–SN hydrogel, (ii) M–DN hydrogel, and (iii) EDS
image of the M–DN hydrogel.

binding mode between CS and MXene was recognized
by FTIR spectra. As shown in Fig. 2(e), the shift in the
–OH characteristic peak from 3,434 cm-1 (red line) to
3,424 cm-1 (blue line) suggests the formation of strong
hydrogen bonding interactions between CS and
MXene [21]. Comparing the MXene sheet modified
with CS to the unmodified MXene after lyophilization,
CS did not affect the overall black color. This means
that CS had essentially no effect on the NIR light
response of the MXene. In addition, the CS-modified
MXene evidently became more compact and difficult
to crush due to the excellent fixation effect of CS
on MXene, which made it difficult to peel (Fig. 2(f)).
After mixing CS–MXene with the prepolymerization
solution, the hydrogel was prepared. The large pores
of several hundred microns inside the single network
hydrogel and double network hydrogel were observed
by SEM. The messy microporous structure of the
single network hydrogel contrasts sharply with the
uniform regular pore structure of the dual network
hydrogel, as shown in Figs. 2(g)–2(i) and 2(g)–2(ii).
This regular pore structure was more conducive
to improve the hydrogel strength and form more
hydrated layers. The EDS analysis showed that the
basic carbon (C) and O elemental distribution was
consistent with the holes. In addition, the Ti elements
did not show large-scale agglomerations, confirming
that the modified MXene was more uniformly
dispersed.
3.2 Characterization of the mechanical properties
of M–DN hydrogels
The PNIPAM component in the M–DN hydrogel acted
as both a ductile substance and a molecular chain in

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response to temperature stimulation [24]. Therefore,
the strength of the M–DN hydrogels was subject to
changes in by temperature. The tensile strength of
the M–DN hydrogels at different temperature was
tested using a universal mechanical testing machine.
As shown in Figs. S4(a) and S4(b) in the ESM, the
M–DN hydrogel had strength of 0.2 MPa at room
temperature. The PNIPAM network in the hydrogel
underwent a phase change when heated to 50 °C.
Meanwhile, the molecular chains contracted, resulting
in poor ductility. Therefore, the stress and strain of
the M–DN hydrogel were reduced but still remained
at 0.15 MPa (Fig. 3(a)) [30]. The compressive strengths
of the M–SN and M–DN hydrogels were tested to
reveal the compression condition during the friction
process. The results showed that the M–DN hydrogel
had a strong compression resistance of 1.0 MPa, which
far exceeded the strength of the M–SN hydrogel and
was sufficient to guarantee its strength for use at low
loads (Fig. 3(b)). To further investigate the strength
differences between the single and double network
hydrogels, rheological tests were carried out on the
M–SN hydrogels and M–DN hydrogels. The energy
storage modulus (G') and loss modulus (G") of the
double network hydrogels were both an order of
magnitude higher than those of the single network,
exhibiting greater energy dissipation and use strength
(Fig. 3(c)).
To measure the phase change temperature of
the M–DN hydrogels, a temperature scan of their
mechanical properties was carried out by using a
rheometer. The sudden rise in G" at approximately
40 °C confirmed that PNIPAM underwent a phase
change and molecular chain contraction. It transformed
from the hydrophilic state to hydrophobic state at this
point, which provided a reference for the subsequent
frictional regulation of the temperature inflection point
(Fig. 3(d)). In addition, the hydrogel's resistance to both
tensile and compressive processes was accompanied
by covalent bond breakage, which was a major
challenge for the versatile applications of the hydrogel.
Ten loading–unloading tensile tests at 30% strain were
carried out on M–DN hydrogels at room temperature.
The stresses and strains remained essentially
unchanged, indicating good resilience with little
breakage of covalent bonds under these tensile strain
conditions (Fig. S5(a) in the ESM). Then, loading–
unloading compression tests were carried out at

Fig. 3 Characterization of the mechanical properties of M–DN hydrogels. (a) Results of tensile strength at break of the M–SN
hydrogel and M–DN hydrogel at 25 and 50 °C, respectively; (b) comparison of the compressive strength of M–SN hydrogels with
M–DN hydrogels; (c) comparison of the energy storage modulus and loss modulus of the M–SN hydrogel and M–DN hydrogel;
and (d) variation in the energy storage modulus and loss modulus of the M–DN hydrogel from 25 to 50 °C.

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different strains (15%, 18%, and 20%). It was evident
that the compression strength decreased from 0.29 to
0.2 MPa (approximately 69.0% of the original value)
as the number of cycles increased after 10 cycles
of the 15% strain test. As the strain increased, more
covalent bonds were broken. The magnitude of this
change increased sequentially but remained high
compressive strength (Figs. S5(b)–S5(d) in the ESM),
which endowed the M–DN hydrogel with high
strength to prevent breakage in friction applications.
3.3 Near-infrared photoresponse properties of M–DN
hydrogels
The MXene nanosheets in the M–DN hydrogel
conferred unique NIR photoresponsiveness to the
hydrogel. As shown in Fig. 4(a), the hydrogel was
placed in a petri dish with the addition of an
appropriate amount of water. It was found that the
response temperature showed a gradient increase for
different concentrations of MXene nanosheets doped
into the hydrogel. M–DN hydrogels were stimulated
by NIR light before and after the response. It could
be visually observed that the M–DN hydrogel became
whitish from a completely transparent state, and the
water spilled around it. This phenomenon occurred
because the PNIPAM molecular chain became
hydrophobic and contracted, destroying the surface
as well as the internal hydration layer of the hydrogel
(Fig. 4(b)).
The effects of the MXene nanosheet concentration
and NIR light intensity on the M–DN hydrogels
were further evaluated. As shown in Fig. 4(c), the
temperature of five different concentrations of MXene
nanosheets under NIR light irradiation was tested. The
results showed that the changing rate of temperature
and final value increased with concentration of MXene
nanosheets. Then, the effects of different irradiation
powers on the M–DN hydrogel (0.8 mg/mL) were
explored. Figure 4(d) shows that both the changing
rate of temperature and the final value increased
with power, even reaching over 80 °C at 2.0 W/cm2.
Combined with the previous rheological tests, it

Fig. 4 NIR photoresponse properties of M–DN hydrogels. (a) Infrared thermal images of M–DN hydrogels with different MXene
nanosheet concentrations and different NIR light irradiation times; (b) schematic diagram of the M–DN hydrogel response and optical
images before and after the response; (c) temperature curves of M–DN hydrogels with different MXene nanosheet concentrations as a
function of irradiation time at NIR light irradiation power of 1 W/cm2; (d) temperature versus time curves for 0.8 mg/mL M–DN
hydrogels irradiated with different powers of NIR light; and (e) temperature cycling profile of the 0.8 mg/mL M–DN hydrogel under
NIR light irradiation at a power of 1.0 W/cm2.

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Friction 12(1): 39–51 (2024) 47

was concluded that 40 °C was the phase transition
temperature for this system. Thus, an irradiation
power of 1 W/cm2 was selected to modulate the
0.8 mg/mL hydrogel to achieve a fast response and
a low upper limit temperature. Under the above
conditions, the M–DN hydrogel of 0.8 mg/mL was
tested for cycling at NIR light-regulated temperature
with the boundary line of 40 °C. The M–DN hydrogel
could quickly rise above that temperature under NIR
light stimulation, while it quickly cooled to below
40 °C with the help of the surrounding water when
the NIR light was switched off. The phenomenon
remained repetitive under three cycles (Fig. 4(e)), which
achieved a stable and rapid NIR light-stimulated
phase transition.
3.4 Friction-modulated properties of
hydrogels
To investigate the effect of NIR light on the friction
modulation of M–DN hydrogels, the COF of hydrogels
was obtained by a universal mechanical tester
(UMT-3) in reciprocating mode. The glass ball and
the hydrogel were used as the upper and the lower
friction pair, respectively. As shown in Fig. S6(a) in
the ESM, the downwards pressure volume of the
glass sphere was difficult to calculate accurately. The
double network hydrogel was stiffer than conventional
hydrogels. To test the contact area, dye was applied
to the glass spheres. The size of the contact area
between the glass sphere and the hydrogel was tested
indirectly by pressing the glass sphere down onto
the paper on the surface of the hydrogel. As shown
in Fig. S6(b) in the ESM, the contact area was
approximately 3.14 mm2 and was fully covered by
NIR light. As shown in Fig. S6(c) in the ESM, the NIR
light during the experiment was illuminated in a
M–DN circle with a diameter of 1 cm, which was sufficient
to cover the entire test area of 5 mm reciprocating
stroke.
As shown in Fig. 5(a), without the NIR light
irradiation, PNIPAM was hydrophilic. The hydrated

Fig. 5 Friction modulation characterization of MD–N hydrogels. (a) Optical picture of the friction test equipment; (b) COF variation of
M–DN hydrogels under different NIR light power (MXene concentration: 0.8 mg/mL; load: 1 N; frequency: 1 Hz; and amplitude: 5 mm);
(c) effect of different MXene nanosheet concentrations on the COF of M–DN hydrogels (NIR light power: 1.0 W/cm2; load: 1 N; frequency:
1 Hz; and amplitude: 5 mm); (d) variation in three friction-modulated cycles of 0.8 mg/mL M–DN hydrogels (NIR light power: 1.0 W/cm2;
load: 1 N; frequency: 1 Hz; and amplitude: 5 mm); and (e) variations of 0.8 mg/mL M–DN hydrogels with multiple modulated cyclic COF
(NIR light power: 1.0 W/cm2; load: 1 N; frequency: 1 Hz; and amplitude: 5 mm. Error bars = standard deviation, n = 3).

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48
layer on the surface of the hydrogel was the key to
achieve low friction. When the NIR light was turned
on, MXene rapidly responded and generated a large
amount of heat, which raised the temperature of the
hydrogel above the LCST. At this point, PNIPAM
underwent a phase transition into the hydrophobic
state. Consequently, the surface hydration layer was
destroyed rapidly. At the same time, the internal
hydration layer also decreased. These aspects decreased
the friction reduction capacity and thus increased the
COF [27, 31, 32].
Initial tests of the loads and frequencies required for
hydrogel testing were carried out prior to modulation.
The results showed that the COF continued to increase
as the load increased. Even though the double network
hydrogel was still a flexible material, the friction pair
caught in the hydrogel under higher load conditions,
increasing the resistance during friction. The friction
pairs didn’t completely contact at lower load conditions.
Therefore, 1 N was chosen as the load pressure for all
subsequent tests. Friction was unstable both at high
and low frequency conditions. Thus, the tests were
carried out at 1 Hz (Fig. S7 in the ESM). As shown
in Fig. 5(b), the power of the NIR light was adjusted
after the COF was stable for 300 s. The COF of
the hydrogel changed from ~0.02 to ~0.15 with
increasing power. This change rate increased with
power, which was consistent with the previous NIR
light response rate. In Fig. 5(c), the comparison on
the response rates of hydrogels with different MXene
nanosheet concentrations under NIR light (1 W/cm2)
were conducted. It took approximately 100 s to reach
the highest COF for the sample with a 0.8 mg/mL
MXene nanosheet in M–DN hydrogel. It was evident
that the COF of the hydrogel changed more
dramatically under NIR light irradiation with the
increase of MXene nanosheets concentration. Three
successive modulated cycle tests were performed on
0.8 mg/mL M–DN hydrogels under NIR light with
a power of 1 W/cm2. Repeated switching of the NIR
light stimulated the MXene nanosheet response. It
enabled the M–DN hydrogel with the fast transition
between low and high COF. The low and high COF
value always remained approximately 0.02 and 0.135,
respectively. This is because the uniformly dispersed
MXene nanosheets enhanced their utilization, thus
prompting a rapid increase in temperature. The surface
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Friction 12(1): 39–51 (2024)
and a certain amount of internal hydration layer
could be quickly destroyed by the phase transition of
PNIPAM. When the ambient temperature returned to
room temperature after the water loss, PAMPS had
strong water absorption capacity as well as the recovery
of hydrophilicity. The rapid absorption of pure water
in the tank increased the amount of hydrated layer.
As a result, the COF returned to the original value
(Fig. 5(d)). To further verify the modulation stability
of the M–DN hydrogels under 1 N loading condition,
three samples were taken for ten modulation cycles.
As shown in Fig. 5(e), the mean COF value remained
at approximately 0.02 for low values and 0.135 for
high values. It indicated that the M–DN hydrogel
was more stable under 1 N loading condition for
modulation. This confirmed the potential of M–DN
hydrogels as controlled drives, flexible robotic arms,
and gripping soft materials [33].
4 Conclusions
In summary, we achieved the construction of a
well-disperse MXene double-network hydrogel by
incorporating the chitosan (CS) polymer, which
could rapidly responded to the near-infrared light
(NIR light) with good recyclability and controllability.
Poly-N-isopropylacrylamide (PNIPAM) polymer was
selected as the second layer of the MXene dual-network
hydrogel, which could increase both the hydrogel
strength and the sensitivity under the external stimuli.
The thermo-responsive behavior of PNIPAM polymer
endowed the MXene-functionalized PNIPAM/CS
double network hydrogel (M–DN hydrogel) with rapid
transition between the low friction state (μ~0.021)
and the high friction state (μ~0.135) by forming and
disrupting the hydration layer below and above the
lower critical solution temperature (LCST), respectively.
This MXene-based hydrogels show great potential
in friction modulation and intelligent lubrication. In
addition, the high strength of M–DN enabled the
potential application in interfacial sensing, controlled
actuation, and flexible robotic arms.
Acknowledgements
We acknowledge the financial support from the
National Natural Science Foundation of China (No.
Friction 12(1): 39–51 (2024)
52175187), the China Postdoctoral Science Foundation
(2021M692625), and the Fundamental Research Funds
for the Central Universities.
Declaration of competing interest
The authors have no competing interests to declare
that are relevant to the content of this article. The
authors Feng ZHOU and Weimin LIU are the Editorial
Board of Members of this journal.
Electronic Supplementary Material: Supplementary
material is available in the online version of this article
at https://doi.org/10.1007/s40544-022-0726-2.
Open Access This article is licensed under a Creative
Commons Attribution 4.0 International License, which
permits use, sharing, adaptation, distribution and
reproduction in any medium or format, as long as you
give appropriate credit to the original author(s) and
the source, provide a link to the Creative Commons
licence, and indicate if changes were made.
The images or other third party material in this
article are included in the article’s Creative Commons
licence, unless indicated otherwise in a credit line to
the material. If material is not included in the article’s
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not permitted by statutory regulation or exceeds the
permitted use, you will need to obtain permission
directly from the copyright holder.
To view a copy of this licence, visit
http://creativecommons.org/licenses/by/4.0/.
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from Tiangong University and
received his master degree in the
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full professor at Northwestern
Polytechnical University. He received
his BEng. (2009) in materials
chemistry and MEng. (2012) in
materials science from Hubei
University (China). Then, he com-
pleted his Ph.D. (2015) in materials
science under the supervision of prof. Weimin Liu
and prof. Feng Zhou at Lanzhou Institute of Chemical
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Center of Advanced Lubrication and Sealing
Materials in 2023 from Northwestern Polytechnical
University. His research interests include MXene
based composite hydrogels and their intelligent
friction.
Physics, Chinese Academy of Sciences. From 2015
to 2019, he worked as a postdoctoral fellow in the
prof. Zijian Zheng’s group at Hongkong Polytechnic
University. As the first author or corresponding
author, he has published more than 30 peer-reviewed
high-quality papers, such as Chemical Reviews, Advanced
Materials, Nature Communications, and Small. His
research interest includes functional lubrication, bionic
tribology, nanoscale lubricating additives, polymer
science, and 3D nanofabrication.
Friction 12(1): 39–51 (2024)
Feng ZHOU. He is a full professor
in Lanzhou Institute of Chemical
Physics, Chinese Academy of
Sciences, China, and head of
Lanzhou Institute of Chemical
Physics and State Key Laboratory
of Solid Lubrication. He gained his
Ph.D. degree in 2004 and spent three
51
years (2005–2008) in the Department of Chemistry,
University of Cambridge as a research associate. He
has published more than 500 journal papers, which
have received more than 28,000 citations and have
a high-index of 90. His research interests include
bioinspired tribology, biomimic surfaces/interfaces
of soft matter, drag-reduction, anti-biofouling, and
boundary lubrication.
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