Sensors & Actuators: A.

Physical 368 (2024) 115059

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Sensors and Actuators: A. Physical

journal homepage: www.journals.elsevier.com/sensors-and-actuators-a-physical

A strain-resistant flexible thermistor sensor array based on CNT/MXene

hybrid materials for lithium-ion battery and human
temperature monitoring
Baichuan Sun , Gaobin Xu *, Xu Ji , Zhaohui Yang , Cunhe Guan , Shirong Chen , Xing Chen ,
Yuanming Ma , Yongqiang Yu , Jianguo Feng
Micro Electromechanical System Research Center of Engineering and Technology of Anhui Province, School of Microelectronics, Hefei University of Technology, Hefei,
Anhui 230009, People’s Republic of China

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

Keywords: Flexible thermistor sensors (FTSs) are well-suited for myriad applications involving strain and dynamic tem­
Flexible thermistor sensors (FTSs) perature monitoring due to the outstanding thermosensitive performance and flexibility but still challenging. In
Carbon nanotubes (CNTs) this study, a novel FTS is proposed based on the hybrid materials of carbon nanotubes (CNTs) and MXene, in­
MXene
tegrated with an innovative flexible substrate (paper/polydimethylsiloxane (PDMS)/Si3N4 nanoparticles), which
FTS array
achieves low cost, stain resistance and results in a wide temperature detection range (− 20 to 220 ◦ C) with su­
Lithium-ion batteries (LiBs)
Wearable devices perior thermosensitivity (− 0.52% ◦ C⁻1), exceptional temperature resolution (~ 0.3 ◦ C), rapid response and re­
covery times (~300 ms and 3 s, respectively), and excellent mechanical durability (withstanding 2000 bending
fatigue cycles). And the sensors excel in diverse conditions like compression, underwater, and curved surfaces.
Additionally, the optimal thermosensitive performance is achieved with a 1:2 ratio of CNT and MXene. Mech­
anistic analysis reveals that the addition of CNT can effectively adjust the interlayer spacing of MXene, enhancing
its electrical and thermosensitive properties. Furthermore, a 2 × 2 FTS array is successfully applied for
comprehensive temperature monitoring in lithium-ion batteries (LiBs), as well as for monitoring human body and
environmental temperatures as wearable devices. This technology offers high sensitivity and real-time temper­
ature recognition, providing the possibilities for FTS applications in environmental monitoring, medical elec­
tronics, and electric vehicles.

1. Introduction
Temperature, as a fundamental parameter, holds undeniable signif­
icance, playing a critical role in various domains, from ensuring the
safety of LiBs in the rapidly evolving electric vehicle industry to its vital
importance in medical applications, especially in COVID-19, directly
influencing safety and well-being [1–3]. However, conventional rigid
temperature sensors and infrared (IR) cameras exhibit limitations in
achieving dynamic and real-time temperature detection, often suscep­
tible to interference from moving targets, leading to inaccuracies [4,5].
In contrast, flexible temperature sensors, with their inherent adapt­
ability to irregular shapes, have addressed these limitations and are
widely used in wearable devices, electronic skin, environmental moni­
toring, automotive, and aerospace applications [6–8].
Flexible temperature sensor encompasses the flexible thermocouple
sensor (FTCS) [9], the flexible capacitive thermistor sensor (FCTS) [10],
the flexible infrared sensor (FIRS) [11], and the flexible thermistor
sensor (FTS) [12]. While FTMS offers a wider temperature range but
with lower precision, suitable for general low-precision industrial ap­
plications. FTCS has challenges in low-temperature detection, sensi­
tivity, and temperature range. FIRS enables non-contact measurements
but are typically characterized by larger dimensions, rendering them
unsuitable for miniaturization, and are sensitive to ambient temperature
and reflectance. FTS, known for the rapid response times, heightened
sensitivity, and suitability for irregular surfaces, has attracted significant
research attention. However, these sensors face challenges like me­
chanical stress vulnerability and limited temperature measurement
range, driving ongoing research for improvements.
Efforts to achieve superior mechanical performance and precise
temperature measurements have focused on using thermosensitive

* Corresponding author.
E-mail address: gbxu@hfut.edu.cn (G. Xu).

https://doi.org/10.1016/j.sna.2024.115059
Received 24 November 2023; Received in revised form 25 December 2023; Accepted 18 January 2024
Available online 20 January 2024
0924-4247/© 2024 Elsevier B.V. All rights reserved.
B. Sun et al.
nanomaterials, including carbon nanomaterials (CNTs [8,13], carbon
black [14], graphene [15]), MXene [16], and metallic materials (Pt [17],
Ag [18], and Au [19]). Among them, metallic materials are considered
suboptimal due to the high cost, limited stability, and potential envi­
ronmental hazards. In contrast, carbon nanomaterials offer impressive
electrical conductivity, thermosensitivity and a wide operational tem­
perature range but suffer from weak mechanical performance, leading to
delamination and fractures [8]. Conversely, MXene demonstrates
excellent mechanical properties and electrical conductivity. However, it
is susceptible to oxidation and humidity, yet it demonstrates favorable
compatibility when combined with other materials. In this study, we
aimed to develop a novel hybrid material by combining CNT with
MXene, striving to achieve a material that offers exceptional mechanical
performance, excellent thermosensitivity, and a wide temperature
range. Furthermore, the domain of CNT/MXene hybrid materials in the
field of thermistors has been relatively unexplored, and there is a lack of
substantial theoretical groundwork, leaving room for further research
and exploration.
In addition to excellent thermal sensitivity, the FTSs rely on the
flexible substrate for exceptional mechanical performance, enabling
adaptation to irregular shapes, bending, and deformation, reducing the
impact of stress on its performance. Commonly used flexible substrate
for FTS include polyimide (PI) [20], polyethylene terephthalate (PET)
[21], PDMS [22,23], and paper [24,25]. PI and PET, as traditional
polymers, offer exceptional heat resistance and chemical stability.
However, PI faces challenges due to its high production costs and
manufacturing complexities, while PET, in comparison to PI, exhibits
lower heat resistance and mechanical strength and is prone to softening
and deformation when exposed to high temperatures. PDMS, provides
excellent transparency and flexibility but suffers from poor mechanical
properties and high coefficient of thermal expansion (CTE), making it
prone to deformation and detachment of the electrodes [26]. In recent
years, paper has garnered interest because of its remarkable biocom­
patibility, cost-effectiveness, and eco-friendliness. Nonetheless, it does
have certain mechanical limitations and is best suited for single-use
scenarios. To enhance the performance of paper, a common approach
involves combining it with PDMS to improve its hydrophobicity and
mechanical properties [27]. Nevertheless, this method retains the dis­
advantages associated with PDMS. To address these challenges, the
incorporation of nanofillers has become a prevalent choice [27–29]. For
instance, Racles et al. [28] have combined PDMS with Ag nanoparticles,
resulting in a harmonious enhancement of PDMS’s mechanical perfor­
mance while reducing its CTE (in a linear relationship with Ag content)
and achieving a maximum strain of 550%. Suzuki et al. [29] have
effectively lowered the CTE of PDMS by blending it with four types of
silicon nanofillers, with mesoporous silica particles demonstrating
optimal results.
Herein, we employed Si3N4 nanoparticles as nanofillers due to the
excellent high-temperature stability, outstanding mechanical proper­
ties, corrosion resistance, and biocompatibility, which were integrated
with the paper/PDMS composite using a combination of screen printing
and compression techniques, resulting in the topological interlocking
and heterogeneous arrangement that gave rise to the FTS capable of
withstanding deformation and high temperatures. Furthermore, Si3N4
played a crucial role in dispersing stresses and further restraining
deformation [30]. Moreover, the novel hybrid materials of CNT and
MXene exhibited the capability to detect a wide range of temperatures,
spanning from − 20 ◦ C to 220 ◦ C, with excellent thermosensitivity
(− 0.52%℃− 1), remarkable resolution (0.3 ◦ C), and rapid response times
(3 s). Even after enduring over 2000 bending deformations, FTS
continued to perform temperature monitoring flawlessly, with minimal
interference, thus achieving accurate temperature discrimination on
irregular surfaces. Most importantly, the 2 × 2 FTS array has been
successfully integrated into LiBs and wearable devices, meeting the
temperature monitoring needs of LiBs while also detecting temperature
fluctuations in real-time in and around the human body for health
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Sensors and Actuators: A. Physical 368 (2024) 115059
monitoring purposes. We firmly believe that the proposed FTS, not only
fulfills the aforementioned demands but also opens new avenues and
possibilities for more precise temperature monitoring in various fields,
including aerospace, electric vehicles, and medical electronics.
2. Materials and methods
2.1. Materials
Whatman No.1 filter paper was purchased from Whatman Company,
UK. PDMS (Sylgard184) was purchased from Dow Corning, USA. Ag/
Agcl ink and PI film was purchased from Zhuhai Jinshi Energy Tech­
nology Co., Ltd. CNT (In this study, single-walled carbon nanotube
(SWCNT) is employed, which will be refer to as CNT for conciseness
throughout the paper), MXene and Si3N4 nanoparticles were purchased
from beike 2D materials Co., Ltd. Silane coupling agent (SCA) and acetic
acid were purchased from Dongguan Shanyi Plastics Co., Ltd. Screen
printing machine was purchased from Hunan Deyun Printing Equipment
Co., Ltd. Magnetic/electric stirrers, ultrasonic disruptor, constant tem­
perature heating table and vacuum drying oven were purchased from
Lichen Technology Co., Ltd. CCD and microscope were purchased from
Beijing Lepu Technology Co., Ltd. Thermal IR imaging camera was
purchased from Hangzhou MicroImage Software Co., Ltd. Thermostatic
bath (HMDC2006) was purchased by Jiangsu Hengmin Instrument
Manufacturing Co., Ltd. Lithium batteries (LiBs) and battery capacity
testers were purchased from Anhui Sanuo Electronic Technology Co.,
Ltd. Digital multimeter purchased from Future Electronic Technology
Co., Ltd.
2.2. The fabrication process of FTS
To fabricate the FTS, materials need to undergo a series of treat­
ments, as illustrated in Fig. 1(a–c). The initial step involves separately
mixing MXene and CNT powders with deionized (DI) water and the
surfactant through ultrasonic dispersion and stirring to prepare solu­
tions, which are subsequently combined using the same process to
obtain the blended solution. Next, as depicted in Fig. 1(b), the Si3N4
nanoparticles are chemically surface-modified using the SCA (intro­
ducing amino functional groups). This modification serves to establish
not only a physical connection between Si3N4 and PDMS but also a
chemical reaction (amino functional groups, -NH2) that can react with
the silicone-oxygen bonds (-Si-O-) in PDMS, forming silicon-nitrogen
bonds (-Si-NH2) [31]. Furthermore, the enhanced surface roughness of
the modified nanoparticles promotes superior topological interlocking
[32]. Prior to modification, the nanoparticles undergo activation treat­
ment at 120 ◦ C for 2.5 h in the vacuum oven. Next, they are subjected to
ultrasonic and stirring processes in the SCA. Notably, the solution re­
quires the addition of acetic acid to adjust the PH to 5. The mixture is
then left at room temperature for 1 day, followed by centrifugation
(during which distilled water and anhydrous ethanol are separately used
for washing, with three cycles). Finally, the materials are placed in the
vacuum oven at 60 ◦ C for 12 h to yield the surface-modified Si3N4
nanoparticles. The last step (Fig. 1(c)) involves mixing the chemically
modified Si3N4 with PDMS (2.0 wt%), resulting in the necessary solution
for printing.
The experiment uses the screen printing to create the FTS. Custom
screen-printing plates are prepared (Fig. 1(d)) to define the required
patterns. PDMS/Si3N4 is then printed onto paper, requiring multiple
printings for full contact and pattern creation (Fig. 1(d)). This step es­
tablishes hydrophobic and hydrophilic regions, with the latter for
thermosensitive materials. The substrate is heated at 80 ◦ C for 1 h in the
vacuum oven. CNT/MXene hybrid materials are printed in the desig­
nated pattern area (Fig. 1(e)), followed by Ag/AgCl electrode printing
(Fig. 1(f)). Then, the second PDMS/Si3N4 printing (Fig. 1(g)) serves to
encapsulate the CNT/MXene, preventing oxidation upon exposure to air
and acting as a barrier against contaminants. Additionally, the
B. Sun et al. Sensors and Actuators: A. Physical 368 (2024) 115059

Fig. 1. The fabrication process of FTS. (a) Preparation of CNT and MXene blend solution; (b) Surface modification of Si3N4 nanoparticles; (c) Mixing PDMS with
Si3N4 nanoparticles; (d) Screen printing PDMS/Si3N4 on paper; (e) Screen printing of MXene/CNT hybrid materials; (f) Printing the Ag/AgCl electrode; (g) Second
Round of PDMS/ Si3N4 printing; (h) Second encapsulating of FTS using PI film and compression (20 MPa); (i) Cross-sectional image of FTS.

mechanical and thermal properties in this region are enhanced. Simi­
larly, it is heated at 80 ◦ C for 1 h. The final step (Fig. 1(h)) involves
attaching a PI film to the back of the FTS, serving as a secondary
encapsulation and facilitating attachment to the desired location.
Furthermore, it is crucial to subject the completed FTS to compression
(20 MPa, 30 min) to improve the contact, eliminate void between ma­
terial layers, and further enhance mechanical performance. With these
steps, the FTS is completed, and the cross-sectional image is shown in
Fig. 1(i).
2.3. Simulation
Prior to conducting experiments, we performed mechanical and
thermal simulations on the FTS to compare the curved and block
structure and to assess how they respond to external conditions under
identical resistance. SolidWorks was employed for three-dimensional
(3D) modeling, and COMSOL Multiphysics was used for further char­
acteristic analysis.
In the thermodynamic simulation, the boundary conditions for FTS
were established based on the actual testing system and conditions. The
sensitive materials were the CNT/MXene hybrid materials, and the
flexible substrate was considered as a solid block for analysis. The
ambient temperature was set at 25 ◦ C, and the heating temperature was
set at 80 ◦ C, with the bending stress of 10 N/m2. Stress was applied from
both the X and Y directions. As depicted in Fig. 2(a–d), it can be observed
that, under the combined influence of bending deformation and thermal
expansion, the block structure exhibited significantly greater internal
stress compared to the curved structure. Consequently, it was more

3
B. Sun et al.
Fig. 2. Simulation analysis of FTS. (a)-(b) Thermodynamic simulation analysis of curved structure FTS in X and Y directions; (c)-(d) Thermodynamic simulation
analysis of block structure FTS in X and Y directions; (e)-(g) Thermodynamic simulation analysis of Si3N4 in the flexible substrate.
susceptible to deformation and more prone to stress-induced de­
formations. Moreover, the lower CTE of the thermosensitive material, in
comparison to the substrate, aids in mitigating stress concentration
during thermal expansion. Therefore, the adoption of the curved design
enhances the stability of FTS for measuring temperature variations.
Additionally, thermodynamic simulations were performed on the
Si3N4 nanoparticles within the substrate to characterize their role in the
FTS. The 3D structure (10 ×10 ×2 µm3) consisted of two layers, with the
first layer being the CNT/MXene and the second layer as the flexible
substrate. The boundary conditions matched the previously described
setup, with the bottom of the substrate being subjected to fixed con­
straints. As depicted in Fig. 2(e) - (g), it is evident that the presence of
Si3N4 concentrates stress within its own region. This property effectively
disperses in-plane stress concentration, thereby suppressing the defor­
mation and thermal expansion effects. Moreover, due to the low CTE,
high strength, and good thermal conductivity of Si3N4, it further en­
hances the substrate’s mechanical properties, reducing mechanical
deformation and the impact of temperature on the FTS.
3. Results and discussion
3.1. FTS encapsulation and resistance variation
The fabricated FTS in this study is illustrated in Fig. 3(a–c). Fig. 3(a)
shows the FTS without PDMS/Si3N4 encapsulation, featuring the black
pattern representing the CNT/MXene (1:2) hybrid materials, with the
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Sensors and Actuators: A. Physical 368 (2024) 115059
width of 0.5 mm, the bending radius of 0.5 mm, and the approximate
thickness of 0.2 mm. As observed in the SEM image, the CNT/MXene
hybrid materials exhibit the fibrous tubular structure for CNT and the
sheet structure for MXene. CNT primarily consists of C atoms, while the
employed MXene is Ti3C2Tx, composed of Ti, C, Tx (F and O atoms), and
H atoms (Fig. 3(b)). Moreover, Fig. 3(c) reveals that after the second
layer of PDMS/Si3N4 encapsulation, the CNT/MXene is covered
beneath, serving to prevent exposure to contaminants and oxidation
risks. Furthermore, energy-dispersive X-ray spectroscopy (EDS) analysis
in Fig. 3(d) and (e) reveals higher C content, primarily due to the
presence of cellulose fibers in the paper and the inherent C content in
CNT and MXene. Additionally, there are notable amounts of Ti, O, and F
present. In the encapsulated FTS, the introduction of Si and N elements
due to the PDMS/Si3N4 encapsulation is confirmed.
Furthermore, as depicted in Fig. 3(g), the unencapsulated FTS un­
dergo oxidation when exposed to the air, resulting in increased resis­
tance and thus impacting the detection performance. Moreover, this
oxidation process accelerates with rising temperatures. For instance, at
20 ◦ C, after 9 h, the resistance increased by approximately 1%. At 80 ◦ C,
the resistance increased by around 8%. In contrast, the encapsulated FTS
maintains stable resistance at the same temperature conditions. Even
after 30 days of storage at room temperature (Fig. 3(h)), the resistance
remains essentially unchanged. In contrast, the unencapsulated FTS
experiences the resistance change of approximately 7.5%. This clearly
highlights the significance of encapsulation, while also confirming the
convenience and effectiveness of using the same materials in flexible
B. Sun et al. Sensors and Actuators: A. Physical 368 (2024) 115059

Fig. 3. Internal structural analysis and resistance change comparison of encapsulated and unencapsulated FTS. (a) Physical and SEM images of unencapsulated FTS;
(b) Schematic representation of CNT and MXene composition; (c) Physical and SEM images of encapsulated FTS; (d) EDS analysis of unencapsulated MXene; (e) EDS
analysis of unencapsulated CNT/MXene; (f) EDS analysis of encapsulated CNT/MXene; (g) Resistance comparison of encapsulated and unencapsulated FTS under
heating conditions (20–80 ◦ C); (h) Resistance comparison of encapsulated and unencapsulated FTS at room temperature (20 ◦ C) after 30 days of storage.

substrate for this purpose.
3.2. Performance analysis of CNT/MXene hybrid thermosensitive
materials
To determine the optimal performance of CNT/MXene hybrid ma­
terials in thermosensitive applications, we compared different mixing
ratios (4:1, 3:1, 2:1, 1:1, 1:2, 1:3, 1:4). To simplify the fabrication and
observation, we used a 0.5 × 4 mm2 paper along with the thermo­
sensitive materials (Fig. 4(a)). The resistance of CNT and MXene is
48.47 Ω and 194.27 Ω, respectively. Furthermore, we observed varia­
tions in resistance at different mixing ratios. Following mixing, an initial
resistance increase was observed, with a subsequent decline in resis­
tance becoming apparent as the MXene content increased. This behavior
stems from interface effects between MXene and CNT. Limited contact
introduces interface resistance, hindering electron flow and increasing

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B. Sun et al. Sensors and Actuators: A. Physical 368 (2024) 115059

Fig. 4. Performance comparison of the CNT/MXene hybrid materials. (a) Resistance comparison of CNT, MXene, and different mixing ratios; (b) XRD comparison of
CNT/Paper, MXene/Paper, CNT/MXene/Paper, and encapsulated CNT/MXene; (c) Comparison in resistance variation with temperature for CNT, MXene, and
different mixing ratios of hybrid materials; (d) Schematic illustration of the NTC principle for hybrid materials; (e) Comparison of TCR for CNT, MXene, and different
mixing ratios of hybrid materials; (f) Comparative I-V characteristics of hybrid materials at different temperatures (20–80 ◦ C); (g) Resistance variation of hybrid
materials under heating and cooling conditions (− 20–220 ◦ C); (h) Arrhenius plot depicting the linear correlation between ln(R) and temperature (1000/T).

resistance. Simultaneously, fibrous structure of CNT can fill gaps be­
tween MXene layers, reducing electron scattering and enhancing con­
ductivity while lowering resistance [33].
To further substantiate the findings, we conducted X-ray diffraction
(XRD) tests on CNT/Paper, MXene/Paper, CNT/MXene/Paper, and
CNT/MXene/Paper encapsulated with PDMS/Si3N4. As shown in Fig. 4
(b), apart from the three cellulose crystal planes of the paper (101),
(101), and (002) corresponding to angles of 14.9◦ , 16.5◦ , and 22.8◦ , two
crystal planes persisted: CNT’s (100) plane and MXene’s (002) plane,
corresponding to angles of 26◦ and 6.9◦ , respectively. Notably, with the
addition of CNT, the peak of MXene shifted to around 4.6◦ , indicating
that the inclusion of CNT resulted in an increased interlayer spacing in
MXene, corroborating the accuracy of the previously described
observations [33]. Furthermore, it’s worth mentioning that PDMS and
Si3N4 nanoparticles lack specific crystal planes, resulting in the absence
of prominent crystal facets in the XRD analysis.
Additionally, to further compare the performance of materials in
thermosensitive applications, the FTS was attached to the surface of the
thermostatic bath and connected them to the DMM for testing. It’s
essential to note that we assessed the thermal responses by studying the
relationship between relative resistance change (ΔR/R0) and tempera­
ture. In Fig. 4(c), we observed a consistent decrease in resistance for
different materials from 20 ◦ C to 80 ◦ C. This behavior can be attributed
to the negative temperature coefficient (NTC) properties of both CNT
and MXene. As the temperature rises, electrons transition to the con­
duction band, increasing carrier density, which, in turn, reduces

6
B. Sun et al.
resistance (Fig. 4(d)). Notably, when CNT and MXene are combined in a
1:2 ratio, the resistance change is particularly conspicuous. Further­
more, compared to pure CNT and MXene, the hybrid materials exhibit a
faster resistance change within the same temperature range. To evaluate
the role of thermosensitive materials in thermal sensing, the tempera­
ture coefficient of resistance (TCR) was quantified as Eq. (1):
TCR = [(RT − R0 )/R0 ]/ΔT (1)
where RT represents the instantaneous resistance at temperature T, and
R0 corresponds to the initial resistance at the reference temperature
(20 ◦ C). As illustrated in Fig. 4(e), it is evident that the hybrid materials
with the 1:2 mixing ratio exhibit a notable TCR, amounting to − 0.52%
◦ − 1
C , surpassing several literature-reported thermosensitive sensors
with CNT, as shown in Table 1. This further illustrates that the addition
of CNT into MXene fills the interlayer gaps, enhances electrons transi­
tion to the conduction band, increases carrier density, thereby
improving the TCR of the hybrid materials. However, an excess of CNT
can lead to insufficient interlayer contact in MXene, thereby diminishing
the TCR (Fig. 4(e)). Consequently, we adopted the CNT/MXene blend
ratio of 1:2 in our experiments. Moreover, Fig. 4(f) showcases that the
hybrid material maintains a robust I-V relationship with exceptional
ohmic characteristics across various temperatures.
Furthermore, we conducted extensive high and low-temperature
experiments on the FTS, expanding the scope of our investigations, as
shown in Fig. 4(g). Remarkably, over a wide temperature range from
− 20 ◦ C to 220 ◦ C, the change in resistance of the FTS demonstrated an
approximate quadratic relationship, with correlation coefficients (R2)
reaching 0.99 during both the heating and cooling phases. Notably,
cyclic heating and cooling tests revealed nearly overlapping curves,
suggesting minimal hysteresis effects. Given the nonlinear relationship
between resistance and temperature, we utilized the Arrhenius model
(Eq. (2)) to fit the data:
ln(R) = ln(Ri ) + B/T = ln(Ri ) + Ea /2kB T (2)
where Ri signifies the resistance at infinite temperature, Ea represents
the thermal activation energy, kB represents the Boltzmann constant,
and Ea /2kB T=B is referred to as the thermal index (Fig. 4(h)). The strong
linearity observed between ln(R) and 1000/T within the range of − 20 ◦ C
to 220 ◦ C, with an R2 value of 0.97, underscores the dominant role of
thermally activated charge carriers in the Arrhenius-like temperature
dependence, highlighting the pronounced NTC behavior.
3.3. Sensing performance of FTS
To quantitatively analyze the sensing performance of FTS, tests were
conducted under various conditions. Specifically, FTS was attached to
the outer wall of the thermostatic bath and subjected to temperature
changes from 20 ◦ C to 80 ◦ C and from 20 ◦ C to − 20 ◦ C, to evaluate its
response time and recovery time. Typically, response time and recovery
time are determined using the criteria of a 10% and 90% change in
resistance, respectively, to assess the response speed and recovery
characteristics of sensors [13]. As shown in Fig. 5(a), under both heating
and cooling conditions, the response time of FTS was approximately
300 ms, with recovery times of about 3 s and 3.3 s, respectively,
showing minimal differences. Furthermore, to validate the stability of
Table 1
Comparison of sensitivity and detection ranges for different FTS.
Material Sensitivity (℃− 1) Range Ref.
CNT/PET -0.4% -40-100 ℃ [13]
CNT film -0.07% 4.2-420 K [34]
MWCNT/PVBC_Et3N -0.4% 20–40 ◦ C [35]
Epoxy/MWCNT composites -0.036% 20-160 ◦ C [36]
MWCNT/PMMA composites -0.13% 20-160 ◦ C [37]
CNT/MXene/Paper/PDMS/Si3N4 -0.52% -20-220 ◦ C
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Sensors and Actuators: A. Physical 368 (2024) 115059
FTS, multiple thermal cycles (20–90 ◦ C) were performed, and the rela­
tive current change (ΔI/I0) was recorded. As depicted in Fig. 5(b), after
10 cycles, the performance of FTS exhibited negligible variation, making
it suitable for continuous monitoring applications. Additionally, preci­
sion tests were conducted, demonstrating that FTS can accurately detect
resistance changes within around 0.3 ◦ C range (Fig. 5(c)). This illus­
trates the outstanding temperature resolution of FTS, rendering it suit­
able for detecting subtle temperature variations.
To further validate the applicability of the FTS in complex conditions
such as compression, underwater environments, and bending de­
formations, we integrated the FTS with these different scenarios and
conducted reactivity tests by monitoring relative resistance changes
(ΔR/R0). As shown in Fig. 5(d), when subjected to varying levels of
pressure by adding pure water into the beaker (0–44 N), the resistance
remained almost unchanged, indicating its stress-inhibiting character­
istics, which may be related to the topological interlocking between the
substrate materials and stress dispersion of Si3N4 nanoparticles. Sub­
merging the FTS underwater (Fig. 5(e)) and heating it to 90 ◦ C, the re­
sults were nearly identical to those obtained in the air, confirming the
waterproof performance of FTS. In addition, we conducted bending tests
at various angles (from 0 ◦ − 90◦ , Fig. 5(f)). As the bending angle
increased, the resistance also increased. However, at a high angle of 90◦ ,
the relative resistance change did not exceed 0.15%, making it negli­
gible. After undergoing 100, 1000, and 2000 bending cycles, the resis­
tance changes displayed a consistent trend, further verifying the strain
resistance of FTS. Moreover, as shown in Fig. 5(g), the relative resistance
changes at high temperatures (80 ◦ C) remained consistent, even after
numerous deformations. To validate the adaptability of FTS to different
surfaces, as shown in Fig. 5(h), we conducted temperature tests on both
flat and curved surfaces (20–90 ◦ C). The results revealed nearly identical
relative resistance changes. Therefore, the FTS is suitable for most
operating conditions and enables real-time, precise temperature moni­
toring over a wide range.
3.4. Practical applications of FTS
3.4.1. Practical application of FTS in LiB monitoring
Temperature monitoring of LiBs is crucial to ensuring their safety
and efficient operation. To enable real-time temperature monitoring of
the commercial LiB (10 Ah, with dimensions of 110 mm in length,
60 mm in width, and 12 mm in thickness), the thermal IR imaging
camera was used in comparison with the FTS. Furthermore, for the
convenience of data recording, the resistance changes in the FTS were
converted into temperature changes using the linear equation as illus­
trated in Fig. 4(h). In order to further determine the internal tempera­
ture distribution of the LiB during charging, simulation and modeling
were conducted. As shown in Fig. 6(a), it was observed that the tem­
perature surrounding the positive electrode of the battery was higher
than that around the negative electrode, and the central region exhibited
higher temperatures compared to the sides. In pursuit of enhanced
temperature monitoring accuracy and sensitivity, as depicted in Fig. 6
(b), a 2 × 2 sensor array (with dimensions of 60 ×50 mm2) was
employed to facilitate comprehensive analysis and monitoring of the
LiB. The experimental setup for temperature monitoring, shown in Fig. 6
(c), consisted of the FTS, LiB, battery capacity tester, and DMM.
The initial experiment involved charging and discharging the LiB at a
3C rate (9A). Fig. 6(d) and (e) show that the battery generated heat
during these processes, with the discharging process exhibiting slightly
higher temperatures than the charging process. Notably, there was an
initial rapid temperature increase, followed by a period of stabilized
temperature rise, and finally, a rapid increase in heat generation. These
observations are consistent with previous research findings [38].
Importantly, FTS embedded the LiB monitoring results closely aligned
with thermal IR monitoring, affirming the practicality and effectiveness
of the FTS.
Subsequently, we conducted tests using the battery tester at different
B. Sun et al. Sensors and Actuators: A. Physical 368 (2024) 115059

Fig. 5. Sensing Performance of FTS. (a) Resistance changes of FTS under heating (80 ◦ C) and cooling (− 20 ◦ C) conditions; (b) Relative current changes (ΔI/I0) of FTS
after 10 cycles of heating; (c) Resolution of FTS; (d) Resistance changes of FTS under compression (0–44 N); (e) Resistance changes of FTS when heated underwater;
(f) Resistance changes of FTS under bending deformation (No.1, No.100, No.1000, No.2000); (g) High-temperature response of FTS after bending deformation; (h)
Comparative analysis of relative resistance changes with temperature for FTS on different surfaces.

charge and discharge rates, specifically 1C (3A), 2C (6A), 3C (9A), 4C
(12A), and 5C (15A), while recording temperature changes. As depicted
in Fig. 6(f) and (g), as the charge and discharge rates increased, the
temperature rise rate of battery accelerated, accompanied by a corre­
sponding temperature increase. This behavior can be attributed to the
heat generation formula (Q = I2 Rt), where higher current results in
increased heat production, consequently leading to a faster temperature
rise. Furthermore, the heat generated during charging was slightly lower
than during discharging, and both temperature variations followed
linear trends. Specifically, the charging process exhibited an R2 of
approximately 0.99, while the discharging process displayed an R2 of
around 0.96 (with a slight deviation at the 1 C rate, where the R2 was
approximately 0.948).
To further validate the effectiveness of the sensor array and assess
temperature variations at different locations within the battery, we
employed each of the four individual FTS sensors separately. As
observed in Fig. 6(h) and (i), the temperature increase was most rapid
near the positive electrode (Sensor 1), followed by Sensors 2 and 3.
Sensor 4, situated far from the positive electrode and closer to the edge
of the battery, exhibited a temperature difference of approximately 2 ◦ C
compared to Sensor 1. This comprehensive data underscores the ca­
pacity of array for real-time monitoring at distinct locations within the
battery. Moreover, real-time monitoring achieved through flexible
contact enhances methods such as IR monitoring that are unable to meet
the demands of continuous monitoring.

8
B. Sun et al. Sensors and Actuators: A. Physical 368 (2024) 115059

Fig. 6. Physical application of FTS in LiB Monitoring. (a) Schematic diagram of internal temperature distribution within the LiB; (b) Schematic diagram of the FTS
array placed inside the LiB; (c) Monitoring platform for LiB charge and discharge; (d)-(e) Temperature variations during LiB charge and discharge at the 3 C rate,
compared with IR camera monitoring; (f)-(g) Temperature changes during LiB charge and discharge at different rates (1 C, 2 C, 3 C, 4 C, 5 C); (h)-(i) Temperature
monitoring distribution of the array during LiB charge and discharge.

3.4.2. Physical application of FTS in wearable devices
Wearable devices are crucial in temperature monitoring, providing
real-time and convenient temperature data, which is essential for health
and various applications. Therefore, our experiment applies FTS to
temperature monitoring on both the human body and the environment.
In the experiment, the FTS array is placed directly on the skin of the
human arm for monitoring, as depicted in Fig. 7(a), and compare it with
real-time data from the IR imaging camera. As shown in Fig. 7(b) and
(c), the images display the temperature of the arm skin under normal
state and after running, demonstrating that the temperature in the FTS
closely corresponds to that of the arm, highlighting excellent thermal
conductivity. Furthermore, Fig. 7(d) illustrates the temperature from the
four sensors within the array, all exhibiting consistent trends with
temperature differences not exceeding 0.1 ◦ C. These minor differences
may be attributed to the non-uniform temperature distribution on the
human body and transient temperature fluctuations. Additionally, the
average temperature is calculated from the four sensors within the array
and compare them with data from the IR monitoring camera (Fig. 7(e)).
The results reveal that under normal state, the temperature of the arm
remains at approximately 33.3 ◦ C. After physical activity, the temper­
ature increases by approximately 1 ◦ C due to the movement of blood
within the body. And, it returns to its original temperature within half an
hour. The high level of consistency with reference data reaffirms the
effectiveness of the FTS.
Next, we affixed the FTS array onto the surface of clothes to achieve
environmental temperature monitoring, as shown in Fig. 7(f). To

9
B. Sun et al. Sensors and Actuators: A. Physical 368 (2024) 115059

Fig. 7. Practical applications of FTS as a wearable device for human body and environmental temperature monitoring. (a) Physical image of the FTS array in contact
with the arm skin. (b)-(c) IR images of the human arm under normal state and after running. (d) Real-time temperature monitoring comparison of the FTS array’s four
sensors on the arm. (e) Temperature comparisons between FTS and IR camera monitoring under different states. (f) Physical image of the FTS array attached to
clothes. (g) Comparative monitoring of environmental temperature by FTS and an IR camera. (h) Temperature monitoring comparisons at various distances of the
FTS from a heat source.

monitor real-time environmental temperature changes, we deactivated
the lab’s temperature control device, allowing us to observe temperature
fluctuations. The monitoring results from FTS and the IR camera were
almost identical, as depicted in Fig. 7(g). Furthermore, we placed the
FTS array in close proximity to a heat source (50 ◦ C) and observed that
the closer it was to the heat source, the more accurate the temperature
measurements became. When positioned at a 1 cm distance, the moni­
toring accuracy reached 99%. This capability provides FTS with an
application in early heat warning systems. However, at a 10 cm distance
from the heat source, there was still some thermal response, albeit with
reduced accuracy due to heat diffusion and convection effects, providing
a form of temperature warning to a certain extent.
4. Conclusion
In this work, we propose a novel FTS based on hybrid materials of
CNT/MXene, which is fabricated on the flexible substrate composed of
paper/PDMS/Si3N4, enabling accurate real-time temperature moni­
toring and exhibiting resistance to deformation interference. It holds
practical application value in various fields, including LiB temperature
monitoring, human and environmental temperature sensing. Notably,
our research reveals that a 1:2 mixture ratio of CNT/MXene exhibits
optimal performance in the thermosensitive fields. Furthermore, the
proposed FTS is capable of a wide temperature detection range (− 20 to
220 ◦ C) with outstanding thermosensitive properties (TCR=− 0.52%
◦ 1
C⁻ ), remarkable resolution (~0.3 ◦ C), and excellent response and re­
covery times during high and low-temperature cycles (~300 ms and 3 s,
respectively). It showcases superior durability, maintaining accurate
temperature data acquisition even after undergoing 2000 bending cy­
cles. Moreover, it can be applied in various scenarios, including
compression deformation, underwater conditions, and on curved sur­
faces. Additionally, we have successfully applied the 2 × 2 FTS array to
LiB and human/environmental temperature monitoring, particularly as
a wearable device. In comparison to the commercial IR imaging camera,
FTS excels in temperature recognition and overcomes the limitations of
continuous monitoring faced by IR detection. In conclusion, from a
structural perspective, the preparation of the FTS substrate mitigates the
impact of deformation interference in the temperature sensor domain. In
terms of materials, the introduction of a novel hybrid thermosensitive
materials of CNT and MXene offers improved sensitivity and mechanical
performance. Concerning performance, the FTS array achieves high
sensitivity, a wide temperature range, and high-precision temperature
recognition. It can be anticipated that FTS provides a simple, cost-
effective, and efficient method for producing flexible temperature sen­
sors and holds promising prospects in various fields, including aero­
space, electric vehicles, and medical electronics.

10
B. Sun et al.
CRediT authorship contribution statement
Ma Yuanming: Methodology. Chen Xing: Validation, Methodology.
Chen Shirong: Methodology, Investigation, Data curation. Guan
Cunhe: Supervision, Software. Yang Zhaohui: Project administration,
Methodology. Ji Xu: Software, Resources, Methodology. Xu Gaobin:
Visualization, Validation, Investigation, Funding acquisition, Formal
analysis, Conceptualization. Sun Baichuan: Writing – review & editing,
Writing – original draft, Software, Project administration, Investigation.
Feng Jianguo: Visualization, Validation. Yu Yongqiang: Methodology,
Formal analysis.
Declaration of Competing Interest
The authors declare that they have no known competing financial
interests or personal relationships that could have appeared to influence
the work reported in this paper.
Data availability
No data was used for the research described in the article.
Acknowledgments
This research was partially supported by National Key Research and
Development Program of China (2022YFB3205903) and Major R&D
Innovation Project of Anhui Provincial Development and Reform Com­
mission (JZ2021AFKJ0050).
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Baichuan Sun received his B.S., and M.S. degree in School of
Mechanical and Electronical Engineering from Henan Univer­
sity of Technology, Zhengzhou, China. He is currently pursuing
his PhD at the Hefei University of Technology, with my main
research focus on MEMS, flexible sensors, thermal runaway of
lithium batteries and wearable devices, etc.
B. Sun et al.
Gaobin Xu received his B.S. degree from Hefei University of
Technology in 1993, M.S. degree from Hefei University of
Technology in 2001 and Ph.D. degree from Southeast Univer­
sity in 2004. Now he is a professor and Ph.D. supervisor at
Hefei University of Technology. His main research interests
include MEMS sensor design, manufacturing, packaging and
reliability, multi-sensor module integration and information
fusion technology.
Xu Ji received his B.S. degree in School of Science at Yanshan
University in Applied Physics, Qinghuangdao, China. He is
currently pursuing his M.D. at the Hefei University of Tech­
nology, with his main research focus on electrostatic
microspeaker.
Zhaohui Yang received his B.S. degree in School of Mechanical
and Electronical Engineering from Chizhou University, Chiz­
hou, China. He is currently pursuing his PhD at the Hefei
University of Technology, with his main research focus on
MEMS infrared detectors.
Cunhe Guan received his B.S. degree in School of Mechanical
and Electronical Engineering from Chizhou University, Chiz­
hou, China. He is currently pursuing his M.D. at the Hefei
University of Technology, with his main research focus on the
reliability of MEMS devices.
Shirong Chen received her M.S degree in detection technology
and automation from Institute of Intelligent Machines, Chinese
Academy of Sciences in 2006. She is currently a lecturer in
School of Microelectronics, Micro Electromechanical System
Research Center of Engineering and Technology of Anhui
Province, Hefei University of Technology. Her main research
interest is microelec-tronic technology and microelectronic
packaging.
12
Sensors and Actuators: A. Physical 368 (2024) 115059
Xing Chen received his B.S and M.S degree in school of mi­
croelectronics from Hefei University of Technology, Hefei,
China. He is currently working at school of microelectronics,
Hefei University of Technology, Hefei, China. His research in­
terests include MEMS and nMEMS.
Yuanming Ma received his B.S. and M.S. degree in School of
Microelectronics, Hefei University of Technology, Hefei,
China. He is currently a lecturer in School of Microelectronics,
Hefei University of Technology, Hefei, China. His research in­
terests include MEMS sensors and systems.
Yongqiang Yu is currently an associate Professor in School of
Microelectronics, Micro Electromechanical System Research
Center of Engineering and Technology of Anhui Province,
Hefei University of Technology. His main research interests are
low-dimensional semiconductor materials and micro/nano Si-
based infrared photodetectors and its applications in PPG
measurement and single-pixel imaging, and wide band-gap
semiconductors.
Jianguo Feng received his B.S., M.S. and PhD degree in School
of Mechanical Engineering from Northwestern Polytechnical
University, Xi’an, China. He is currently working at School of
Microelectronics, Hefei University of Technology, Hefei,
China. His research interests include microfluidics and
bioMEMS.