Journal of Materiomics 6 (2020) 321e329

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Journal of Materiomics
journal homepage: www.journals.elsevier.com/journal-of-materiomics/

Highly sensitive flexible capacitive pressure sensor with a broad linear

response range and finite element analysis of micro-array electrode
Longquan Ma a, b, Xuecheng Yu a, c, Yuanyuan Yang a, Yougen Hu a, Xinyu Zhang a,
Huayuan Li a, Xing Ouyang b, Pengli Zhu a, *, Rong Sun a, **, Ching-ping Wong d
a
Shenzhen Institute of Advanced Electronic Materials, Shenzhen Institutes of Advanced Technology, Chinese Academy of Sciences, Shenzhen, 518005, China
b
School of Materials Science, Shenzhen University, Shenzhen, 518071, China
c
Shenzhen College of Advanced Technology, University of Chinese Academy of Sciences, Shenzhen, 518055, PR China
d
School of Materials Science and Engineering, Georgia Institute of Technology, Atlanta, USA

a r t i c l e i n f o a b s t r a c t

Article history: With the continuous development of wearable electronics, health care and smart terminals, highly
Received 29 August 2019 performance flexible pressure sensors present a huge application prospect. In this study, by introducing
Received in revised form the micro-array structured electrodes and dielectric layers with high dielectric constant, capacitive
27 November 2019
pressure sensor fabricated with a brand new preparation strategy and highly sensitive is proposed. The
Accepted 20 December 2019
prepared micro-array structure is the basis for sensors with high sensitivity. Besides, the contact area
Available online 27 December 2019
between the two electrodes changes from linear to planar with the increased loading, which result in a
wider linear responding range. In addition, by introducing ceramic dielectric material-barium titanate
Keywords:
Pressure sensor
(BT) fillers into the dielectric layer to increase it’s the dielectric constant, the sensitivity of the sensor
Barium titanate shows two-fold increase. Moreover, the sensitivity gradients can be tuned by changing the loading
Dielectric layer contents of BT particles. Hence, compared with parallel board capacitive sensors with ordinary dielectric
Micro-array structure layer, these sensors exhibit excellent performance as follow, high sensitivity (up to 4.9 kPa
1) under low
Tunable sensitivity pressure range (0e2500 Pa), low detection limit (<1.7 Pa), short response time (<50 ms), a stable
response over 5000 loading-unloading cycles, bending stability and an adjustable sensitivity. Further, the
flexible pressure sensor can detect the pressure of the water droplets and monitor human movement
behavior. With the facile design and excellent comprehensive properties, the flexible pressure sensor
provides a new approach to improve the sensitivity and shows a broad application prospects in the
wearable electronics, health care and smart terminals.
© 2019 The Chinese Ceramic Society. Production and hosting by Elsevier B.V. This is an open access article
under the CC BY-NC-ND license (http://creativecommons.org/licenses/by-nc-nd/4.0/).

1. Introduction rapidly evolving technology areas such as artificial intelligence (AI)

The 21st century is an information age. Information science and
technology have penetrated into all areas of our social life and have
profoundly influenced and changed the global economic structure
and people’s production and lifestyle. The information age is based
on intelligence, all of this is inseparable from the collection and
processing of data, so this is also the era of sensors. Sensors have
been extensively researched in the fields of wearable electronics
[1e5], health care [6e8] and smart terminals [9e11], including
* Corresponding author.
** Corresponding author.
E-mail addresses: pl.zhu@siat.ac.cn (P. Zhu), rong.sun@siat.ac.cn (R. Sun).
Peer review under responsibility of The Chinese Ceramic Society.
and Internet of Things (IoT) technology, as sensors enable context
awareness and data collection, it plays a vital role in AI and IoT
application. So the pressure sensor, as an important sensing
element among various electronic devices, is of more and more
interests, as revealed by recently research.
For the above technology to play a better role in human life,
there are strict requirements for the preparation of flexible pres-
sure sensors with low-cost manufacture and over-all properties.
Currently, a wide variety of sensor models have been proposed to
prepare comprehensive properties pressure sensor, and it can be
divided into capacitive [12,13], piezoresistive [14,15], piezoelectric
[16], and triboelectric [17]. Among them, capacitive pressure sensor
has become the focus of research because of its outstanding per-
formance, such as high stability and short response time. In prin-
ciple, the flexible capacitive pressure sensor is a type of traditional

https://doi.org/10.1016/j.jmat.2019.12.008
2352-8478/© 2019 The Chinese Ceramic Society. Production and hosting by Elsevier B.V. This is an open access article under the CC BY-NC-ND license (http://
creativecommons.org/licenses/by-nc-nd/4.0/).
322 L. Ma et al. / Journal of Materiomics 6 (2020) 321e329
parallel plate capacitor, which has a high stability due to its sand-
wich structure, but its application is limited because of the lack of
the sensitivity. Sensitivity is an important indicator to measure the
performance of the sensor. The capacitance (C) of the capacitive
pressure sensor relies on the relative permittivity (εr), the relative
effective proportion of the two electrodes (A), and the distance
between the two electrodes (d). These parameters will change
when external pressure is applied to the capacitive responsive
flexible pressure sensor, and finally reflected in the change of its
capacitance of the pressure sensor which is the key performance of
the sensor. There are various materials for preparing sensors,
mainly including the preparation of flexible electrodes and
dielectric layers. A commonly used material for preparing the
flexible electrodes is via introducing the conductive fillers into the
flexible polymer matrix to result flexible conductive nano-
composites. The most popular flexible polymer substrates include
PDMS, polyurethane (PU), poly (styrene-block-butadien-styrene)
(SBS) [18e20], while the metal particles, metal nanowires and
graphene is the commonly used conductive fillers [2,21e23]. For
the dielectric layer, such as polyvinylidene fluoride (PVDF), methyl
methacrylate (PMMA), polyvinylpyrrolidone (PVP) and Ecoflex sil-
icone elastomers etc, [24e27] those polymer materials with high
dielectric constant are mostly used. In addition, preparation of
composite materials and microstructure construction by using
materials such as polyvinylidene fluoride-trifluoroethylene (P(VDF-
TrFE)), barium titanate (BaTiO3), conductive polyurethane (PU),
multi-walled carbon nanotubes (MWCNTs) and graphene, is also
applied to energy harvesting and highly sensitive self-powered
sensing [28e31].
Around the above mechanism, researchers around the world
have carried out many pioneering works on the improvement of
the sensitivity of capacitive pressure sensors from the following
aspects. Mainly includes structural optimization of the electrodes
and dielectric layers. The reason is that the deformation of the
micro-array structure electrode and dielectric layer increase under
the same pressure conditions which will result in an increase in
sensitivity. Micro-array electrodes has been prepared in a variety of
shapes and preparation methods, such as microstructure of pyra-
mids [32], nanowires [20,33], replicating the microstructure of the
plant surface (rose petal, mimosa leaves etc.) [8,34], “balloon-
blowing” method [35] etc. These have been demonstrated to be an
effective way to improve the sensitivity. Another method is to
process the dielectric layer. On the one hand, the deformation of the
dielectric layer may cause a change in its dielectric constant. On the
other hand, the deformation of the dielectric layer may also cause
the distance between the upper and lower electrodes to change.
Both of these will affect the capacitance of the capacitive pressure
sensor. Bao et al. [36,37] proposed to prepare a pyramid-shaped
dielectric layer by using an etched silicon wafer as a template
with a sensitivity of 0.55 kPa
1. They then combined the pyramid
structure with the air gap to increase the sensitivity to 1.5 kPa
1.
Chen et al. [12] prepares a dielectric layer with holes by adding
ammonium bicarbonate (NH4HCO3) to PDMS substrate, which
greatly improving the sensitivity of the sensor. Regarding the
physical separation of sensors, Ruth and Luo et al. solve this prob-
lem by tightly combining the micro-structured dielectric layer and
the electrode [38,39]. However, the dielectric constant will inevi-
tably decrease while the pores are introduced, the initial capaci-
tance and signal-to-noise ratio will also decrease. The above
research on capacitive pressure sensors mainly focuses on the
geometric optimization of electrodes and dielectric layers. How-
ever, few researchers have focused on how to change the compo-
sition of the sensor’s dielectric layer. In principle, the dielectric
constant of dielectric layers is also an important factor which can
affect the capacitance of the sensor.
Herein, we present a high sensitivity flexible pressure sensor
with micro-array structure electrode and high dielectric constant
dielectric layer. The PDMS substrate is used as top/bottom electrode
by spraying gold, PDMS with micro-array structure is used as bot-
tom electrode. The flexible micro-array structure is obtained by
plasma treatment under low-pressure air, the prestretched PDMS
film shows spontaneous buckle surface structure and is used as the
mold. By using the mold, liquid PDMS is transferred in the micro-
array substrate and established the elastomeric electrode. To
obtain the dielectric layers with high dielectric constant, Barium
titanate with high dielectric constant was added to polyvinylidene
fluoride (PVDF) and mixed well by ball milling method. And the
liquid mixture was spin-coated on the plate PDMS electrode, sub-
sequently. Then, a new design strategy for fabricating capacitive
pressure sensors with both high-sensitivity and wide-working-
range is proposed, by integrating wave-like electrode architecture
with high dielectric permittivity composites. The combination of
micro-array structure electrode architecture and dielectric layers
with high dielectric permittivity demonstrated significant
improvement in both sensitivity and linear-working range, other
than this, the resulting pressure sensor also has a low detection
limit, short response time, high stability and will have an extensive
applications.
2. Experimental section
2.1. Materials
PDMS feedstock was purchased from Dow Corning, Sylgard 184.
DMF was purchased from aladdin with the purity of 99.99%. PVDF
was purchased from Sigma-Aldrich with the Mw of 200000. BT was
purchased from SINOCERA.
2.2. Fabrication of top/bottom electrode
The top/bottom electrode was prepared by gold spraying pro-
cess. In order to prepare PDMS substrate, liquid PDMS precursor
and curing agent are fully mixed in a weight ratio of 10:1, the
bubbles of the mixture was removed by vacuuming or standing a
while about 15 min. Then, the mixture was spin-coated onto a glass
substrate and cured at 70  C for 2 h. To prepared the flat plate gold
electrode, the prepared PDMS substrate was cut into the desired
shape and then spraying gold by putting it in a magnetron sput-
tering apparatus for 100 s. To prepared the micro-array structure
electrode. The cured PDMS was stretched to 130% by using a tensile
clamp and treated with Plasma for 10 min, then released to its
original length to obtain the micro-array structure. The liquid PDMS
mixture was spin-coated onto the micro-array structure PDMS
substrate and cured at 70  C for 2 h. After that, the cured PDMS and
the micro-array structure substrate are separated to obtain a flex-
ible micro-array structured substrate. Subsequently, the flexible
micro-array structure electrode was obtained by spraying gold for
100 s. Finally, the top/bottom electrodes are cut to the desired size
for the experiment.
2.3. Preparation of the dielectric layer loading with different
content of BT and pressure sensor
The process of preparation the dielectric layer loading with
different content of BT was executed as follows, the PVDF powder
matrix was first mixed with different content of BT nanoparticles
and then the mixture is dispersed in DMF solvent at a concentration
of 100 mg/ml. Four different BT content solutions were configured
and mixed well by ball milling method. After standing a period of
time, the solution was spin-coated onto the flat electrode by spin-
 L. Ma et al. / Journal of Materiomics 6 (2020) 321e329
coating, and then kept in an oven at 60 for 8 h to form a film and to
be in close contact with the flat-plate electrode. Finally, the micro-
array PDMS electrode was laminated onto the flat-plate electrode
with different dielectric layer to fabricate the flexible capacitive
pressure sensor.
And the top/bottom electrodes are cut into 1*2.5 cm2 (the
effective contact area is 1*2 cm2 except for some area used as
electrode) for the next experiment. The thickness of dielectric layer
is about 50 mm tested by helical micrometer.
2.4. Characterization and measurements
The PDMS film was treated by Plasma etching machine (Dienei
Femto) to obtain the micro-array structure. The dielectric layer was
obtained by ball mill method. The conductive layer of plate elec-
trode and microstructure electrode was obtained by ion sputter
device. The microstructures of the micro-array electrode and
dielectric layer with different content of BT were observed by field-
emission scanning electron microscopy (FEI Nova Nano SEM 450)
and atomic force microscopy (AFM, BRUKER). ZHIQU (model: ZQ-
21B-1) precision instruments with a z-axis motor stage was used
to apply pressure onto the flexible pressure sensor. The capacitance
values were measured by the Instek LCR-6002 m and transmitted to
the data acquisition software (Labview 2016). The linear motor
(LinMot-PS01) is used for cyclic pressurization test.
3. Results and discussion
The capacitive flexible pressure sensor was fabricated as sche-
matically illustrated in Fig. 1. The pressure sensor mainly contents
three parts: the plate PDMS substrates (top electrode), micro-array
PDMS substrates (bottom electrode) and dielectric layers with
tunable dielectric constant. The plate PDMS electrode was simply
prepared by the gold spraying process as shown in Fig. 1a. The pre-
cured PDMS film was placed in an ion sputtering instrument 2 min
to get a plate PDMS electrode. The micro-array PDMS electrode was
Fig. 1. Fabrication process of the capacitive flexible pressure sensor with tunable sensitivity gradients. (a) Schematic of the preparation process of the plate PDMS electrode and
dielectric layer; (b) Schematic of the preparation process of micro-array PDMS electrode; (c) Schematic diagram of sensor pressurization process (d1: initial thickness of dielectric
layer, d2: initial height of micro-array structure, d’1: dielectric layer thickness after compression, d’2: microstructure height after compression).
323
obtained by a transferring process as shown in Fig. 1b, the PDMS
film was first stretched by the stretching device and treated by air
flow plasma, and then the PDMS film was released to its initial
length to form the micro-array structure. The principle that the
microstructure can be formed is that after the plasma etching
process, the surface of the PDMS generates a layer of silicon oxide
(SiOx). The PDMS substrate returns to the original length due to the
release of the tensile force, and the stiff silicon oxide layer will form
a buckled structure during the relaxation. However, as the micro-
array structure is rigid, if used as a pressure sensor directly, it is
prone to damage and form cracks during test. So, the micro-array
PDMS was used as a template, liquid PDMS was dripped onto it
and distributed evenly by spin coating. The liquid PDMS was cured
and stripped from the mold to obtain the flexible micro-array
PDMS substrate, and then used as an electrode after spraying
gold. To obtain the dielectric layers with high dielectric constant,
different amount of BT nanoparticles was added to polyvinylidene
fluoride (PVDF) and mixed well by ball milling method. Later, the
liquid mixture was spin-coated on the plate PDMS electrode to
construct the BT/PVDF dielectric layer with different dielectric
constant. After drying, the micro-array structure electrodes were
stacked onto the plate PDMS electrode with high dielectric constant
dielectric layer to form a flexible pressure sensor. The variation of
the prepared flexible pressure sensor during operation is as shown
in Fig. 1c, and the pitch of the upper and lower electrodes is
reduced, resulting in an increase in the capacitance of the sensor.
The reduction of the electrode spacing includes the compression of
the dielectric layer and the deformation of the electrode micro-
structure. The PVDF dielectric layer is flexible, thickness of the
dielectric layer changes from d1 to d’1 when pressed, but its
compressible range is small because of because of the high Young’s
modulus (>1000 MPa) and Poisson’s ratio (>0.4) of PVDF. The
micro-array structure can provide a large deformation during
compression, the thickness of the micro-array structure changes
from d2 to d’2 under pressure, but it is still not enough to make the
sensor have a high sensitivity. For the above case, we chose to add
324 L. Ma et al. / Journal of Materiomics 6 (2020) 321e329
high dielectric constant material barium titanate to the dielectric
layer to make the sensor with a high sensitivity, and the response
range is also clear increased and stable.
The micro-array PDMS electrode and high dielectric constant
dielectric layer with different content of barium titanate were
characterized by Atomic force microscopy (AFM) and scanning
electron microscopy (SEM) in Fig. 2 and Fig. S1. The three-
dimension (3D) morphology of the micro-array structure repre-
sented from the AFM is shown in Fig. 2a. We can clearly see the
micro-array structure is formed well, the width and height is about
1.9 mm and 0.4 mm, respectively. The SEM plane and cross-section
figures further reveal the morphology of the micro-array structure.
From Fig. 2c-d, the surface of the entire microstructure is
smooth and has a regular shape. The inset of Fig. 2c shows the
wavelength of the micro-array structure is consistent, with an
average size of 1.8 mm, nearly constant with the AFM result, and the
same situation appears in the illustration of Fig. 2d. In a word, the
micro-array structure is uniformed in shape, which ensures the
high sensitivity and stability of the flexible pressure sensor. The
dielectric layer consisting of PVDF and PVDF with different content
of barium titanate is shown in Fig. S1. The thickness of the film is
approximately 40 mm, which is obtained by controlling the spin
speed. The figures show that white particles are uniformly
distributed in PVDF film. The aggregation has started to occur when
the content of barium titanate reaches 30 wt% in PVDF film. It can
be obtained that when the content of barium titanate is further
increased in the PVDF film, the film will not be formed, or the film
has non-uniformity, which will affect the stability of the sensor.
For the variable gap type capacitive sensor, the dielectric con-
stant is positively related to the capacitance value of the sensor, and
the sensitivity of the sensor could be tailored by adjusting dielectric
constant of the dielectric layer of the sensor. Here, BaTiO3
Fig. 2. Microscopic characterization images of the micro-array structure. (aeb) AFM images of the PDMS micro-array mold; (ced) SEM images of the flexible micro-array structure
and the cross-section shape of the PDMS electrode, illustration shows the wavelength of the micro-array structure.
nanoparticles (BT), a well-known dielectric ceramic, are used as the
fillers to improve the permittivity of the dielectric layer, and study
the relationship between the sensor performances and dielectric
constant of the dielectric layers. The frequency dependence of
dielectric properties of the BT/PVDF nanocomposites with different
BT loading were studied by a broadband dielectric spectroscopy at
room temperature. As shown in Fig. 3a, the dielectric constant of
the BT/PVDF nanocomposites present slightly increase in compar-
ison with the corresponding pure PVDF film over a wide range of
frequency (1 kHz to 1 MHz). The pure PVDF film has dielectric
constant about εr ~6.8 at 1 kHz. After introducing 10 wt%, 20 wt%,
30 wt% BT nanoparticles, its dielectric constants increase to 7.8, 9.3,
12.4 at 1 kHz, respectively. This demonstrates that the dielectric
constant of the PVDF film can be increased by adding the high
dielectric constant material, and the dielectric constant is positively
related to the addition contents of the filler. By regulating the
amount of filler amount, the dielectric constant of the inner
dielectric layer can be tailored. Moreover, the content of BT nano-
filler has a little effect on dielectric loss, all the nanocomposite film
maintains a low dielectric loss at frequency below 100 kHz (see
Fig. S2). When the frequency exceeds 1 MHz, the dielectric loss of
the composite film with higher content of nanofiller is increased.
This is because there is an interface between PVDF particles and
barium titanate nanoparticles, resulting in an increase in leakage
current, the rate of dielectric loss under high frequency shows an
upward tendency with the barium titanate content increases. In
general, BT is very useful for increasing the dielectric constant of
the PVDF film, and the dielectric constant of the PVDF film is
increased as the amount of BT added increases. However, the film
formation of PVDF film would be affected if the content of BT were
more than 30 wt%, so in the following sensor fabricated process and
performance evaluating experiments, the maximum BT loading is
 L. Ma et al. / Journal of Materiomics 6 (2020) 321e329 325

Fig. 3. Dielectric constant of the dielectric layer and relative capacitance changeepressure curves for the capacitive pressure sensor. (a) Frequency dependence of dielectric constant
of BT/PVDF nanocomposite films with different BT nanoparticles loading weight fractions; (bec) Relative capacitance change-pressure curves for the capacitive pressure sensors
based on PVDF dielectric layer with different content of BT; (d) Response of the pressure sensor under gradient pressure; (e) Pressure response and relaxation time of the pressure
sensor; (f) Relative capacitance change-pressure curves from a consecutive loading-unloading cycle.

set at 30 wt%.
Subsequently, these dielectric layers with different contents of
BT are applied to the sensor to characterize the performance of the
sensor and investigate the influence of dielectric constant of the
dielectric layer on the performance of capacitive pressure sensor.
For example, pressure sensitivity, hysteresis and response time are
the most important performance parameters for the pressure
sensor.
Firstly, to get the pressure sensitivity, different external pressure
is respectively applied onto the capacitive pressure sensors with
different dielectric constant dielectric layers under the same test
conditions. From Fig. 3b, it can be seen that based on the micro-
array electrodes, the sensor’s pressure response range can be
divided into two linear sections: low pressure range (0e2.5 kPa)
and high pressure range (2.5e10 kPa). Under low pressure range,
the pressure sensitivity of pressure sensor with pure PVDF as
dielectric layer is 1.93 ± 0.16 kPa
1. With gradually increasing the
dielectric constant of the inner dielectric layer, sensitivity of the
pressure sensors increases to 3.08 kPa
1 (PVDF þ 10% BT),
4.07 kPa
1 (PVDF þ 20% BT), 4.9 kPa
1 (PVDF þ 30% BT), respec-
tively. Under high pressure range (2.5e10 kPa), the pressure
sensitivity with different dielectric layer were 0.35 ± 0.07 kPa
1
(pure PVDF), 0.42 kPa
1 (PVDFþ10%BT), 0.48 kPa
1 (PVDFþ20%BT),
0.71 kPa
1 (PVDFþ30%BT). Compared with the sensor sandwiched
with pure PVDF dielectric layer, the sensitivity of the sensor with
high dielectric constant dielectric layer is significantly increased
over the entire pressure response range. These results indicate that
the dielectric constant of dielectric layer has a significant influence
on the sensitivity of the capacitive pressure sensor, and the sensi-
tivity have improved much by introducing dielectric layer with
high dielectric constant. Fig. 3c further shows the effect of high-k
dielectric layer on sensor sensitivity at low pressure range
(0e2.5 kPa). It can be seen that the sensor responds linearly within
the low-pressure response range and has a significantly higher
sensitivity than the high-pressure response range, and could reach
to 4.9 kPa
1 as introducing dielectric layer with dielectric constant
of 12.4 at 1 kHz. However, due to if further increasing the BT content
in the dielectric layer in this experiment, it will affect the integrity
and mechanical properties of the dielectric layer, so the highest BT
loading is kept at 30 wt%, but this provided a new suggestion for
subsequent experiments that we can obtain higher sensitivity of
the sensor by adjusting the dielectric constant of the dielectric
layer.
Capacitive pressure sensor response at gradient pressures are
collected and plotted in Fig. 3d. The relative capacitance remained
almost unchanged when external pressure was applied or not onto
the sensor, the loading and unloading process lasts 1 s during the
experiment. The weights with different weight (100 Pa/250 Pa/
500 Pa) were quickly placed on the capacitive pressure sensor
when need to pressurize, it can be seen that the sensor respond
immediately without any time delay. Similarly, when pressure re-
lief is required, the weight was quickly removed and the sensor
responds rapidly. For the pressure sensor with pure PVDF dielectric
layer, when a 2 g weight (100 Pa) quickly placed on the sensor at
1.0 s, the relative capacitance changes immediately from 0 to 0.32 at
1.10 s and then relative capacitance changes remain stable. On the
contrary, at 2.0 s, when taking the weight from the sensor, the
relative capacitance quickly reduces to 0 at 2.10 s. As the weight of
the same weight loaded on the sensor, the relative capacitance
changes keep all the same. Repeat the above operation and apply
weights of different weights could obtain the gradient pressure
response of the sensor. While for the pressure sensor fabricated
using the 30 wt% BT/PVDF as dielectric layer, the step response was
more pronounced. When 100 Pa, 250 Pa and 500 Pa weights are
loaded onto the two sensors with different dielectric layers (pure
PVDF and 30% BT/PVDF dielectric layer), the response values of the
sensors are 0.29 (pure PVDF), 0.51 (30% BT/PVDF); 0.69 (pure
PVDF), 1.19(30% BT/PVDF); 1.27(pure PVDF), 2.41(30% BT/PVDF),
respectively. The reason for the large difference in response values
is that the dielectric constant of the pure PVDF film is only 6.8, but
326 L. Ma et al. / Journal of Materiomics 6 (2020) 321e329
the dielectric constant of the 30% BT/PVDF film is 12.4. It can be
intuitively seen that the response of the sensor with a higher
dielectric constant dielectric layer is significantly higher.
Throughout the loading-unloading process, the relative capacitance
change of the pressure sensor is almost entirely the same under the
uniform pressure, and the response of the sensor under different
pressures also conforms to the results in Fig. 3d, it is indicated that
the pressure sensor under static pressure has an excellent stability.
Pressure response and relaxation time of the pressure sensor is
shown in Fig. 3e and its insets. The value of the relative capacitance
is basically stable when there is no pressure applied to the sensor,
but when an external pressure (500 Pa) is applied to the sensor at
1.65 s, the relative capacitance variation increased from 0 to 2.2 at
1.7 s and then remains stable. Soon the pressure is unloaded at
3.35 s, the relative capacitance variation decreases quickly return to
0 at 4.05 s. The results show that the response time of the sensor is
less than 50 ms. Fig. 3f exhibits the pressure response of the
pressure sensor during one loading-unloading process. In the
pressure range of 0e10 kPa, a total of 30 pressure values are
selected during the loading process, and the response is recorded.
Subsequent, during the unloading process, the corresponding
response are verified. The result shows that the response of the
sensor to the same pressure during the loading and unloading
process is almost identical, which indicates that the pressure sensor
has no obvious hysteresis.
Fig. 4a shows relative pressure change response of pressure
sensor whether the initial state of the sensor is consistent with the
response after 1000 bending cycles. After 1000 times bending test,
the response value of the sensor is almost unchanged under the
same pressure. This is mainly due to the PDMS substrate and
flexible micro-array structure, which guarantees repeatable
bending stability of the sensor. The inset of Fig. 4a shows the pre-
pared sensor owns excellent bendability. As shown in Fig. 4b, by
loading cyclic pressure for 5000 times, the response stability of
pressure sensor under is measured, and the corresponding relative
capacitance variation is recorded. The circulating pressurization
system includes a multimeter, a linear motor, and a PC device (see
in Fig. S3). Among them, the linear motor is the core for setting the
magnitude and frequency of the applied pressure. During the
experiment, by adjusting the height of the platform of the linear
motor, the pressing device applies pressure to the sensor on the
platform, and the pressing frequency is 1 Hz. During the loading
process, the relative capacitance of the sensor changes from 0 to
Fig. 4. (a) Response consistency of the sensor after 1000 cycles bending test and the illustration is a curved sensor; (b) Response stability of the sensor after 5000 cycles pres-
surization test and the inset of the start and final nine cycles.
1.08, and then the relative capacitance changes to 0 after unloading
process. More than 5000 load-unload cycles were applied to the
sensor and the results are collected and shown in Fig. 4b. Inset of
Fig. 4b shows the initial nine cycles of the loading process and nine
cycles of the final phase, which exhibits that the magnitude of the
response is essentially constant. It can be seen that during the
entire pressurization cycle process, the same pressure is applied
and the response of the sensor is consistent. Thus, the above results
demonstrate that the sensor possesses high response stability
during the repeated loading/unloading and bending process.
Without considering the dielectric layer, the sensitivity of the
capacitive pressure sensor at low pressure is determined by the
variation of the distance between the two plates. To understand the
working mechanism of the capacitive pressure sensor with wave
microstructure, the gap variation between the two layers during
the loading process is observed in Fig. 5a-c. As the pressure in-
creases, the flexible microstructures deform, and the spacing be-
tween the two plates decreases significantly. When the pressure
increases to a certain degree, the deformation of the microstructure
is no longer apparent, resulting in a decrease in the sensitivity of
the pressure sensor. Therefore, the sensitivity of the sensor de-
creases from low pressure to high pressure, which comply with the
experimental results within the entire pressure response range.
Fig. 5c shows the finite element analysis of the wave microstructure
electrode during operation. The result shows that the wave
microstructure has good stability in microstructure deformation
and recovery during work engineering. Generally, for capacitive
pressure sensor, the sharp structures are beneficial to enhance the
sensitivity due to the significant reduction in the spacing of the two
plates under small forces. However, the sensitivity of the pressure
sensor displays a sharp decrease because of the stress concentra-
tion. Stress concentration has a greater influence on the linear
response of the sensor. For sharp microstructures, such as pyra-
mids, the sensitivity when pressed is high, but the linear response
range is generally only about 1 kPa [40]. For hemispherical micro-
structures, there is also significant stress concentration when
pressed, and the linear response range is generally around 400 Pa
[41]. In the wave-shaped microstructure prepared in this paper,
when the pressure is applied, the change of the contact surface is
from the line contact to the surface contact, and at the same time,
due to the structure being smooth, the device has high stability, and
it is not easy to generate damage during the test. Therefore, it has a
large linear response range (over 2.5 kPa) at low pressure. As a
 L. Ma et al. / Journal of Materiomics 6 (2020) 321e329
Fig. 5. Working mechanism of the micro-array structure electrode. (aec) Simulation results of the wave microstructure compression process under 1000 Pa, initial state (a), middle
state (b), End of the compression (c); (d) Characterization of the wave microstructure of three-dimensional stress analysis under 2000 Pa; (e) Contact surface topography of the
micro-array structure electrode.
result, considering the linear range and sensitivity, the wave
microstructure is a better choice.
To illustrate the wide linear response range of the wavy
microstructure, in Fig. 5d-e, we further analyzed the wave micro-
structure of the pressure sensor. Fig. 5d shows the three-
dimensional stress analysis of the wave microstructure under
pressure. It can be seen that when the microstructure is deformed,
the contact surface changes from line contact to surface contact.
Fig. 5e directly shows a certain stage in the process of compression
and the shape of the contact surface. For the variable gap type
capacitive sensor, the ratio of capacitance change to initial capaci-
tance is:
ε0 A
C¼d
1
εr1 þ εdr22
DC C
C0 d ε þ d2
¼ ¼ 1 r2
1
C0 C0 d11 εr2 þ d2
d1 represents the height of the microstructure, d2 represents the
thickness of the dielectric layer, and d11 represents the thickness of
the microstructure after compression. It can be seen from Equation
(2) that in the case where the thickness and permittivity of the
dielectric layer permittivity are constant, the response value of the
sensor will increase as the microstructure variable increases. It is
known that when the wave micro-array structure is pressed, the
contact surface is like a rectangle. This is why the linear response
range of the wave microstructure is higher than other sharp
microstructure. The detection limit of the sensor is an another
important performance indicator of the sensor. Here, we measure
the detection limit of the sensor by detecting the response of the
sensor to a drop of water which is intended to reflect the sensor’s
response of small pressure changes. As shown in Fig. 6a, the water
droplets are dripped onto the sensor at a constant rate through a
5 ml dropper. A drop of water discharged was weighed to about
0.034 g, the speed of the water drops is about 2 s. The area of the
sensor used in the test is 1*2 cm2. According to the pressure for-
mula P ¼ F/S, the pressure of a drop of water is about 1.7 Pa, so the
327
minimum detection limit of the sensor we prepared is less than
1.7 Pa. During the process of the water droplets, the response of the
sensor caused by the pressure of each drop of water is nearly the
same, which demonstrates that the response of the sensor to water
droplets is fully stable. Fig. 6b shows a linear fit of the sensor’s
response to small pressures. The linear fit result is exactly the same
as the sensor sensitivity shown in Fig. 4a. For a flexible pressure
sensor with a 30 wt% BT dielectric layer, the sensitivity at low
pressure (0e2.5 kPa) is measured up to 4.9 kPa
1 in the test, and
the linear relationship of the water drop experimental fit is:
y ¼ 0.00492x-0.00322, this indicates that the sensitivity of the
sensor is 4.92 kPa
1. This further demonstrates the stable linear
response of the pressure sensor at lower pressures. To further
illustrate the sensor’s response to the water drop signal, water
(1) droplets are injected into the container above the sensor through a
syringe, and the same volume of water is injected into the container
at different speeds. The change of the capacitance of the sensor
during the drop of the water drop is recorded and compared.
(2) During the experiment, the purpose of the syringe pump is to drop
the water in the syringe into the container above the sensor, a
schematic diagram of the test device is shown in Fig. 6c. Three
experiments were performed with an infusion rate of 12 ml/min,
18 ml/min, 24 ml/min. Make sure that the volume of water in the
syringe is more than 2 ml for each experiment. Collect the change in
capacitance of the sensor as the water droplets are added to the
sensor within 10 s. The change of the capacitance is measured by
the digital multimeter, then transferred to Labview software
(sampling interval: 100 ms). The test result is shown in Fig. 6d.
Excluding the multimeter to measure the fluctuation of the
capacitor itself, it can be seen that the capacitance values at the
beginning and the end of the sensor at different speeds are the
same. That is, 2 ml of water drops completely to the top of the
sensor container, the sensor capacitance changes are also certain.
On the one hand, this shows that the sensor has good response
stability. On the other hand, 2 ml of water is about 2 g, the size of
the sensor is 1 cm  2 cm, the pressure (P ¼ F/S) is about 100 Pa,
and when the drop velocity is 12 ml/min, a response of more than
20 step signals. As for the impact of water droplets, drip rate of
24 ml/min, 2 ml water could be completely dropped above the
328 L. Ma et al. / Journal of Materiomics 6 (2020) 321e329
Fig. 6. Application experiments of the pressure sensor. (a) Sensor response to ultra-low pressure; (b) Linear response of sensors under ultra-low pressure; (c) Schematic diagram of
a water droplet experimental setup; (d) Capacitance sensor response at different water drip speeds (black: 12 ml/min, red: 18 ml/min, blue: 24 ml/min); (eef) Real-time variation of
the normalized relative capacitance. Insets: Optical photographs showing the movement of the elbow joint (e) and knee joint (f).
sensor in the first 6s, so in the subsequent 4 s, the sensor capaci-
tance values are not significantly reduced, the experimental pro-
cess is not affected by the drop impact. Water drop experiments
reflect the sensor performance well, such as the stability of the
sensor and an excellent response to small pressure.
In principle, specific joint or muscle movement are directly
related to the changes of its longitudinal contraction or elongation
and associated expansion of the cross-sectional area. Based on this
principle, the sensors have a capacity to precisely track minute
changes of the local skin interfacial pressure. The performance
curve of the sensor is obtained by connecting the sensor to the knee
and elbow. As shown in Fig. 6e, the sensor is fixed at the elbow joint
by the wristband. The tester performs normal elbow bending mo-
tion. The bending angle of the elbow is about 0e135 , and the
corresponding response (DC/C0) of the sensor is about 0e3.81. The
test monitoring the knee joint motion is collected and shown in
Fig. 6f. The sensor is attached to the knee joint, and the sensor’s
response is measured when the tester is straightening and bending
the knee. During the test, the knee bend angle is about 0e90 . The
response of the sensor (DC/C0) is between 0 and 1.72. The results
show that the sensor can respond well to the bending signal, and
the response size is proportional to the bending angle, the response
value of the sensor increases as the bending angle increases. The
results of multiple measurements also show that the sensor’s
response to the bending signal is very stable.
4. Conclusions
In summary, we demonstrated a new strategy to make high-
sensitivity pressure sensors resembles a sandwich structure and
controllable dielectric layer, and can be mounted onto biological
skin for behavioral monitoring. PVDF was employed as the polymer
matrix which has a dielectric constant εr ~7, by adding high
dielectric constant of barium titanate, the dielectric constant of the
dielectric layer is improved. we can obtain different sensitivity
gradients of the pressure sensor while the dielectric layer with
different levels of barium titanate. The pure PVDF film and PVDF
film with 10 wt%, 20 wt%, 30 wt% barium titanate have dielectric
constants εr ~6.8, 7.8, 9.3, 12.4, the sensitivity of the pressure sensor
were 2.09 kPa
1 3.08 kPa
1, 4.07 kPa
1, 4.9 kPa
1 under low pres-
sure (0e2500 Pa), respectively. In addition, because of the uncon-
spicuous stress concentration of the wave structure, the sensor has
alarge linear response range with high sensitivity. As a result, such
sensors exhibit good performance, high sensitivity in low pressure
(0e2.5 kPa), low detection limit (<1.7 Pa), short response time
(<50 ms), long-term cycle stability and bending stability. Due to its
excellent performance, the flexible pressure sensor shows a broad
application prospects in the wearable electronic devices and smart
terminals.
Author contributions
All authors have given approval to the final version of the
manuscript.
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.
Acknowledgement
This work was financially supported by National Natural Science
Foundation of China (21571186), National key R&D project from
minister of science and technology of China (2016YFA0202702),
Shenzhen Basic Research Plan (JCYJ20170818162548196). Youth
Innovation Promotion Association of the Chinese Academy of Sci-
ences (2017411).
Appendix A. Supplementary data
Supplementary data to this article can be found online at
https://doi.org/10.1016/j.jmat.2019.12.008.
 L. Ma et al. / Journal of Materiomics 6 (2020) 321e329 329

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