Sensors and Actuators A 285 (2019) 67–72

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Sensors and Actuators A: Physical

journal homepage: www.elsevier.com/locate/sna

A flexible ionic liquid-polyurethane sponge capacitive pressure sensor

Xiaofeng Yang, Yishou Wang, Hu Sun, Xinlin Qing ∗
School of Aerospace Engineering, Xiamen University, Xiamen, 361005, PR China

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

Article history: A flexible microfluidic polyurethane sponge super-capacitive pressure sensor is developed to measure
Received 25 July 2018 the pressure. The innovative sensor contains a polyurethane sponge filled with ionic liquid dielectric
Received in revised form 7 October 2018 layer, and coated with two indium tin oxide polyethylene terephthalate (ITO-PET) films on the top and
Accepted 28 October 2018
bottom, respectively. When external pressure is applied on the sensor, the contact area between ITO-
Available online 2 November 2018
PET electrode and ionic liquid polyurethane sponge (ILPU) dielectric layer increases and the distance
between two ITO-PET electrodes decreases due to the structural deformation, resulting in the capaci-
Keywords:
tance of the sensor increasing rapidly. The external pressure will be determined based on the change
Flexible
Ionic liquid of capacitance. Comparing to traditional pressure sensor, the developed sensor provides a high sensi-
Capacitance tivity up to 5.28 nF/KPa and rapid dynamic responses for pressure measurement. Experiments are also
Deformation conducted to investigate the influence of the temperature and humidity.
Pressure sensor © 2018 Elsevier B.V. All rights reserved.

1. Introduction insensitive, unstable and difficult to reproduce, which hinder their

Flexible electronic sensors with a high deformability and con-
formability are highly desirable in portable and foldable devices
[1–4]. Among the various types of electronic sensors, pressure sen-
sors are one of the most concerned types of sensors since they
serve as fundamental components of a wide range application, such
as folding wing airplane [5,6], soft robotics [7–9], electronic skins
[10,11] and biological sensing [12–15]. In general, there are four
kinds of sensing mechanisms for pressure sensors, including tran-
sistor [16,17], piezoresistance [18–20], piezoelectricity [21,22] and
capacitance [23,24]. Traditional sensors relying on silicon-based
materials have high sensitivity and have been widely applied, but
they are rigid and therefore unsuitable for flexible devices [25,26].
Recently, several flexible pressure sensors have been proposed,
including those based on flexible dielectric layer capacitor [27,28],
reversible microfluidic piezoresistors [29,30] and novel nanomate-
rial sensor [31–33].
Piezoresistive sensors, which transduce the pressure applied
on the sensor to resistance signal, have been widely used owing
to their feasible preparation, low cost and easy signal analysis.
Recently, carbon nanotube [34,35], metallic nanowires [36,37],
novel 2D materials [38,39], conductive porous sponge [40,41], or
conductive fluidics [42,43] are often used as the sensing materi-
als for piezoresistive sensors. However, these sensing materials are
∗ Corresponding author.
E-mail address: xinlinqing@xmu.edu.cn (X. Qing).
application in some specific applications, such as biological sensing.
Relying on the charge accumulation during mechanical deforma-
tion, piezoelectric sensors can achieve high sensitivity and enable
self-powered application [44,45]. However, piezoelectric sensors
can be only used to sense dynamic pressure.
Conventionally, capacitive pressure sensors respond to the pres-
sure applied on sensors with the increase of capacitance due to
the decrease in distance between electrodes and the increase
in effective permittivity of dielectric layer between electrodes
[46,47]. However, the sensitivity of capacitive pressure sensors is
low because of the limited compressive strain and high Young’s
modulus of the solid dielectric elastomer layers. To improve the
sensitivity, wrinkly electrodes and pyramidal elastomer dielec-
tric layers have been used for increasing the deformation of the
elastomer dielectric layers [36,48]. Although higher sensitivity can
be obtained, but the sensitivity decreases rapidly as the applied
pressure increases and the fabrication process of the sensor is
complicated. Porous elastomers or composite porous elastomers
have been also used for improving the sensitivity of the capacitive
pressure sensor [49,50]. Nevertheless, the sensitivity is still low.
Recently, a new method was reported for manufacturing capaci-
tive sensors with high sensitivity [51,52]. The method introduces
dielectric hydrogels layer to form interfacial capacitance electri-
cal double layers. However, they are generally expensive and the
manufacturing process is complicated. Therefore, there is an urgent
need to develop a new flexible pressure sensor with sufficient sen-
sitivity in board pressure regimes. Based on the need, a flexible
microfluidic capacitive pressure sensor is developed to measure

https://doi.org/10.1016/j.sna.2018.10.041
0924-4247/© 2018 Elsevier B.V. All rights reserved.
68 X. Yang et al. / Sensors and Actuators A 285 (2019) 67–72
Fig. 1. Flexible ionic liquid polyurethane-sponge capacitive pressure sensor. (a) Chemical structure of ionic liquid. (b) Schematic diagram of the flexible sensor. (c) Microstruc-
ture of the polyurethane-sponge with ionic liquid dielectric layer.
the surface pressure of a complex structure [53]. However, the sen-
sitivity of sensor at low pressure is much lower than that at high
pressure, which could limit its applications.
In this paper, a high flexible microfluidic super-capacitive
pressure sensor with sensitivity and rapid dynamic response is
developed. The sensor consists of a Polyurethane (PU) Sponge
filled with ionic liquids, and coated with two indium tin oxide
polyethylene terephthalate (ITO-PET) films on the top and bottom.
Experiments are also conducted to study the influence of the tem-
perature and humidity. In addition, the developed flexible sensor
is tested to detect the finger tactile pressure with high sensitivity
and resolution.
2. Experiment
2.1. Materials and apparatus
Polyurethane Sponge (Dongguan Yuan Yuan Sponge Products
Co., Ltd.) was employed in experiment. Ionic liquid 1-butyl-
3-methylimidazolium bis-(trifluoromethyl)-imide (99%, Shanghai
Chengjie Chemical Co. Ltd.) was selected as the sensing material.
Polyethylene terephthalate (PET) coated with 100 nm thick layer
indium tin oxide (ITO, South China Xiangcheng Technology Co. Ltd.)
was used for electrode layer. The double-side adhesive (VHB 4905,
3 M) was selected as the bonding layer.
Scanning electron microscopes (SEM, SUPRA 55, ZEISS,
Germany) was used to observe the microstructure of polyurethane
sponge. Capacitance measurements of sensor were performed on
a WK6500B impedance analyzer (Shenzhen Wenke Electronics Co.,
Ltd.). A KD-II 10/100 N (Shenzhen Kaiqignali Technology Co., Ltd.).
Mechanical testing apparatus was used for precisely applying the
pressure load on the sensor. A temperature and humidity incu-
bator (Shanghai Baixin Instrument and Equipment Factory) was
used to control the testing environments including temperature
and humidity.
2.2. Sensor design
In order to achieve a reversible ionic liquid-ITO electrode con-
tact, surface modification technique was adapted to enhance the
ITO electrode surface hydrophobicity. A fluorinated separation
layer of trimethoxysilane with a proportion of 3% in IPA was
spin at 3000 rpm for 40 s to coat the ITO electrode, and dried at
atmospheric pressure in an oven at 80◦ for 1 h. The ionic liquid
polyurethane sponge (ILPS) dielectric layer was fabricated by coat-
ing ionic liquid onto the backbone of polyurethane sponge through
solution dipping. In order to avoid overflow of ionic liquid, the
polyurethane sponge was pressed under a certain level of pressure
and the excessive ionic liquid was absorbed by napkin. The bonding
layer was attached on the ITO electrode to make a sensing chamber
with an area of 10 mm × 10 mm. The ILPS dielectric layer was trans-
ferred into the sensing chamber and sealed it with another ITO–PET
electrode. Two copper wires connected on the top and bottom sur-
face ITO electrical by conductive epoxy were used to record the
capacitance variation under external pressure. The dimension of
the sensor was 20 mm × 20 mm × 0.6 mm. The chemical structural
of the ionic liquid, schematic diagram of the sensing device and the
microstructure image of ILPU dielectric layer are shown in Fig. 1.
2.3. Sensing principle
The schematic of proposed flexible ILPU capacitive pressure sen-
sor is shown in Fig. 2. The sensing principle of proposed sensor is
based on the interfacial capacitance between ITO-PET electrode and
ILPU dielectric layer, an ultrahigh unit-area capacitance forming
by electrons on the electrode and the counter ions from the ionic
liquid at a nanoscopic distance [54]. Under an external pressure,
the contact area between ITO-PET electrode and ILPU dielectric
layer will increase and the distance between two ITO-PET elec-
trodes decreases due to the structural deformation, resulting in
rapid increase of the capacitance of the sensor.
According to the classical fibrous assembly compression theory,
the relation between the external pressure and capacitance of the
sensor can be describe as [54,55]:
1
P 3
C = C0 A( − ˛f03 )
E
where C is the capacitance of sensor, P is the pressure applied on
the sensor, A is the sensing area, ␣ denotes the parameter associ-
ated with the shape of pores, E and f0 are the porosity and Young’s
modulus of the dielectric layer, respectively.
3. Results and discussions
3.1. Relation between capacitance of sensor and pressure applied
In order to control the load precisely, a computer-controlled step
motor with a spatial resolution of 500 nm was used to apply load
on the sensor, and the load was measured by a force gauge of a
1/2500 N resolution. The sensor used for testing was fixed on an
 X. Yang et al. / Sensors and Actuators A 285 (2019) 67–72 69

Fig. 2. Sensing principle of the flexible ionic liquid polyurethane-sponge capacitive pressure sensor. (a) No external pressure applied on the sensor. (b) Pressure applied on
the sensor. (c) Equivalent circuit model of the sensor.

acrylic plate. In order to perform experiment in the lab, an insu- Table 1

Comparison of the sensitivity of capacitive pressure sensors.
lated plate is attached on the top ITO-PET membrane to convert
a concentrated load into a distributed load to simulate the uni- Types Dielectric layer Sensitivity Sensing Range
form distributed pressure applied on the sensor. To characterize Liquid metal-based Microfluidic [56] 0.26%/10 ␮␧
4
0-3*105 ␮␧
the sensor sensitivity, a load was applied to the center of the insu- Air [57] 0.64%/N 0-1 N
lated plate. The pressure was calculated by dividing the load by Silicon-based Air [58] 3.47 fF/KPa 0-30 Kpa
the area of the sensing chamber. The experimental setup and the Elastic material-based PDMS [37] 7.2 pF/KPa 0.5-2.5 KPa
CNT/PDMS [48] 0.55 nF/KPa 0-0.03 KPa
schematic illustration of load applied on the sensor were shown in
Pyramid PDMS [27] 18.6 fF/KPa 0-2 KPa
Fig. 3(a)-(b). Porous PDMS [59] 0.1 pF /KPa 0-0.02 KPa
In order to demonstrate the repeatability of the sensors, three Microfluidic-based Hydrogel [52] 0.1 pF/kPa 0-40 KPa
samples with the thickness of sensing membrane at 50 ␮m and Nanofiber [55] 114 nF/Kpa 0-1 KPa
PU sponge [this work] 5.28 nF/kPa 0-118 KPa
sensing area at 10 mm × 10 mm. When the pressure was applied
on the sensors, the capacitance of sensors was measured by the
impedance analyzer in real-time with a voltage of 1 V at a frequency
of 100 Hz. Note that, the parasitic is ignored in this work, because is because the ionic liquid generally has a high boiling point, low
the capacitance of the electrical double layer is 1000 times higher vapour pressure and stable conductivity.
than that of the traditional parallel-plate sensor and the relation- The flexibility of sensor allows it to conform readily to curved
ship between capacitance change and pressure is only measured surface. A flexible capacitive sensor was attached on a circular tube
[52]. The slope rate of the curve was defined as the sensing sensitiv- with 20 mm in radius to investigate to the influence of bending on
ity. Fig. 3(c) illustrates the measurements of capacitance of sensors the pressure measurement. As shown in Fig. 3(e), when the exter-
with different pressure applied on the sensors. It is clear that the nal pressure applied on the sensor, the capacitance of the sensor
change of capacitance depends on the pressure. Once the pressure increases rapidly. The sensing sensitivity is 5.77 nF/KPa when the
is applied on the sensor, the ILPU dielectric layer is compressed and pressure is below 116 kPa, which is stable compared with the one
the contact area of ILPU dielectric layer and ITO-PET film increases, measured on the plane.
and capacitance increases. The average sensitivity of the three sen- Quasi-static cycling load with a maximum pressure of 10 K Pa
sors is 5.28 nF/KPa, 5.03 nF/KPa and 5.19 nF/KPa when the pressure at frequency 0.05 Hz was applied on the sensor. The capacitance of
is below 118 K Pa. Both the sensitivity and sensing range of the sensor and pressure applied were recorded, as shown in Fig. 3(f).
sensors is much higher than most of existing capacitive sensor sum- Both capacitance and pressure curves are stable, and they match
marized in Table 1. When the pressure is continuously increased, each other well. It is observed that once the pressure is applied on
the sensitivity decreases due to the reduced mechanical deforma- the sensor, the capacitance increases immediately and the capac-
tion of the ILPU dielectric layer, where the deformation approaches itance is back to the original value after unloading the pressure.
the limitation, and the contact area of ionic liquid PU sponge and Overall, the sensor is able to respond well to the static and dynamic
ITO-PET film increases barely. pressure applied on it.
To check the reliability of senor, a sensor was tested right after
manufacturing and one month later under the same condition. As 3.2. Effect of the temperature and humidity
shown in Fig. 3(d), the properties of the sensor were stable within
a period of one month. The sensitivity of sensor right after manu- The environment of the sensor in service is very complex,
facturing is 5.28 nF/KPa, and it is 5.32 nF/KPa one month later. That humidity and temperature varies in time. Due to the high boiling
70 X. Yang et al. / Sensors and Actuators A 285 (2019) 67–72

Fig. 3. Characterization of the pressure sensing performance of the flexible ionic liquid polyurethane-sponge capacitive sensor. (a) Experimental system for applying pressure
and measuring capacitance. (b) The schematic illustration of load applied on the sensor. (c) Capacitance of the sensor as a function of different pressure. (d) The sensor was
tested right after manufacturing and one month later under the same condition. (e) The relationship of the change in capacitance of the sensor attached on a circular tube
and pressure applied. (f) The relationship of pressure and capacitance of the sensor cyclically compressed by 10 K Pa.

Fig. 4. Effect of the environment factors. (a) Curves of capacitance vs frequency at temperature range from 25 ◦ to 60 ◦ . (b) Curves of capacitance vs frequency at humidity
range from 40% to 80%.
 X. Yang et al. / Sensors and Actuators A 285 (2019) 67–72
Fig. 5. Wearable sensor for finger pressure sensing. (a) Plots showing the relative changes in capacitance of the sensor when it was subjected to dynamic pressing and
releasing cycles. (b), (c) The actual sensor was attached on the index finger.
point, low vapour pressure and non-flammable of ionic liquid, the
environmental temperature fluctuation only poses minor influence
on the interfacial capacitance. As shown in Fig. 4(a), the capaci-
tances of sensor were measured at the temperature range from
25◦ to 60◦ . It is clear that the capacitance increases slowly, and
with a sharp at 50◦ , and then increases faster. At the temperature
below 50◦ , the capacitance is stable with less than 2% variation. This
is likely due to the stabilization of physical and chemical proper-
ties of the ILPU dielectric layer and the ionization of ionic liquid in
the temperature range. When continuously increasing the temper-
ature, EDL capacitance rises faster, it may be due to the increase in
ionization of ionic liquid and the phase transform of the PU sponge
with the temperature above 50◦ .
Furthermore, the performance of the sensor at different humid-
ity level was also investigated. As shown in Fig. 4(b), the capacitance
is very stable at different humidity level ranging from 20% to 80%.
This is because the ionic liquid does not react with water at low-
voltage AC signal and the ionization of ionic liquid is not sensitive
to the humidity.
3.3. Flexible sensors for tactile sensing
An essential function of electronic skin is to translate haptic
perception, such as finger pressure and lateral motion sensing. To
demonstrate the high sensitivity and flexibility of the developed
sensor, it was utilized to measure the finger tactile pressure. As
shown in Fig. 5(b)-(c), the sensor was attached on the index finger
to record the finger pressure. When the sensor was subjected to a
cyclical finger tactile pressure, the capacitance was measured by
the impedance analyzer in real time. As shown in Fig. 5(a), the sen-
sor is sensitive to the finger pressure. When pressure is applied on
the sensor, the capacitance increases immediately and the capaci-
tance variation is positive correlated with the pressure applied on
the sensor. The capacitance of the sensor returns to its initial state
rapidly when pressure is released. Importantly, by repeating the
same pressure for numerous times, the stability of the sensor is
demonstrated.
Apart from finger pressure, due to the high degree of flexible
of the developed sensor, it can be utilized to detect other types
mechanical force, such as stretching force and bending force.
4. Conclusions
A flexible polyurethane-sponge with ionic liquid super-
capacitive pressure sensor was developed. The sensor contains a
71
polyurethane sponge filled with ionic liquid dielectric layer, and
coated with two indium tin oxide polyethylene terephthalate (ITO-
PET) films on the top and bottom. Experimental results show that
the sensor responds well at both static and dynamic pressure with
high sensitivity, up to 5.28 nF/KPa, as well as good linearly and
repeatability. The temperature and humidity effect on the perfor-
mance of senor were also investigated. The capacitance of sensor
with selected materials is stable below 50◦ , and not sensitive to
humidity. Overall, the developed innovative sensor has significant
potential for the low cost and reliable tactile pressure measure-
ment.
Acknowledgements
The authors are grateful for the support by the National
Natural Science Foundation of China (No. 11772279) and the
National Key Research and Development Program of China (No.
2016YFF0203002).
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Biographies
Xiaofeng Yang, received his B.Sc. degree in 2013 from Jiangsu University of Science
and Technology, Zhenjiang, China, the M.Sc. degree from Xiamen University, Xia-
men, China, in 2016. Currently, he is a Ph.D. candidate in Xiamen University. His
main research interests include advanced sensing technology.
Yishou Wang, received his B.Sc. and Ph. D. degrees from Dalian University of Tech-
nology, Dalian, China, in 2002 and 2008, respectively. Now, he is an associate
professor in Xiamen University, Xiamen, China. His main research interests include
structural health monitoring and advanced sensing technology.
Hu Sun, received his B.Sc. and Ph. D. degrees from Nanjing University of Aeronautics
and Astronautics, Nanjing, China, in 2007 and 2014, respectively. Currently, he is an
assistant professor in Xiamen University, Xiamen, China. His main research interests
include structural health monitoring and flexible sensor.
Xinlin Qing received his M.Sc. degree in 1991 from Tianjin University, Tianjin, China,
the Ph.D. degree from Tsinghua University, Beijing, China, in 1993. Currently he is
a distinguished professor in Xiamen University, Xiamen, China. His main research
interests include structural health monitoring and advanced sensing technology.