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Large-Area Compliant, Low-Cost, and Versatile Pressure-

Sensing Platform Based on Microcrack-Designed Carbon
Black@Polyurethane Sponge for Human–Machine
Interfacing
Xiaodong Wu, Yangyang Han, Xinxing Zhang,* Zehang Zhou, and Canhui Lu*

Piezoresistive sensors, which transduce

It is a challenge to manufacture pressure-sensing materials that possess pressure into a resistance signal, are widely
flexibility, high sensitivity, large-area compliance, and capability to detect both used because of their cost-efficient fabrica-
tiny and large motions for the development of artificial intelligence products. tion, easy signal collection, and potential
Herein, a very simple and low-cost approach is proposed to fabricate versatile high pixel density. Conventionally, elasto-
meric conductive composites are proved to
pressure sensors based on microcrack-designed carbon black (CB)@polyu-
be optional sensing materials for piezore-
rethane (PU) sponges via natural polymer-mediated water-based layer-by- sistive sensors.[10–12] However, these mate-
layer assembly. These sensors are capable of satisfying the requirements of rials are insensitive, unstable, and inca-
ultrasmall as well as large motion monitoring. The versatility of these sensors pable of detecting low pressures (<10 kPa,
benefits from two aspects: microcrack junction sensing mechanism for tiny approximating gentle touch).[13] Recently,
delicate and rational assembling of micro/
motion detecting (91 Pa pressure, 0.2% strain) inspired by the spider sensory
nanoconductive materials has attracted
system and compressive contact of CB@PU conductive backbones for large much attention in manufacturing highly
motion monitoring (16.4 kPa pressure, 60% strain). Furthermore, these sen- sensitive pressure sensors, including
sors exhibit excellent flexibility, fast response times (<20 ms), as well as good assembling polyaniline nanofibers and
reproducibility over 50 000 cycles. This study also demonstrates the versatility Au-coated polydimethylsiloxane (PDMS)
of these sensors for various applications, ranging from speech recognition, micropillars,[14] sandwiching ultrathin
gold nanowire-impregnated tissue paper
health monitoring, bodily motion detection to artificial electronic skin. The
between PDMS sheets,[15] hierarchically
desirable comprehensive performance of our sensors, which is comparable to compounding polyurethane (PU) fiber,
the recently reported pressure-sensing devices, together with their significant nylon fiber, Ag nanowires, and piezore-
advantages of low-cost, easy fabrication, especially versatility, makes them sistive rubber,[1] etc.[2] On the other hand,
attractive in the future of artificial intelligence. unique microstructure design has been
demonstrated another effective strategy
for fabricating pressure sensors with high
sensitivity, such as micropyramid array,[16]
1. Introduction hollow-sphere microstructure,[13] porous structure,[17] inter-
locked microstructures[18] and fractured microstructure,[19] and
Flexible and sensitive pressure sensors have considerable scien- so on.[5] Despite these achievements, widespread application of
tific, technological, and commercial impact in various applica- the aforementioned pressure sensors is limited by their sophis-
tions, such as sport motion monitoring,[1] speech recognition,[2] ticated fabrication processes and the use of expensive materials
robot prosthesis,[3] electronic skin,[4] portable healthcare moni- (graphene, silver/gold nanowires, or nanoparticles, etc.). With
tors,[5] etc. In recent years, various pressure-sensing mechanisms the rapid development of artificial intelligence, massive sensor
including transistor sensing,[6] capacitive sensing,[7] piezoelectric materials will be demanded in the near future. Therefore, large-
sensing,[8] triboelectric sensing,[9] especially resistive sensing,[10–19] area compliant and cost-efficient fabrication of sensitive pres-
have been developed to construct sensitive pressure sensors. On sure-sensing materials still remains a great challenge.
the other hand, rational micro- or nanostructural design also plays Spiders are the most sensitive species to surrounding vibra-
an important role in fabricating innovative pressure sensors. tion in the animal kingdom.[20] Their most important vibra-
tion detector is based on a crack-shaped slit system near the
X. Wu, Y. Han, Dr. X. Zhang, Z. Zhou, Prof. C. Lu leg joints between metatarsus and tarsus bones. Inspired by the
State Key Laboratory of Polymer Materials Engineering spider’s sensory system, various crack-based sensors have been
Polymer Research Institute of Sichuan University developed in recent years, including gas sensors,[21,22] torsion
Chengdu 610065, P. R. China sensors,[23] and particularly strain sensors.[24–29] For instance,
E-mail: xxzwwh@scu.edu.cn; canhuilu@scu.edu.cn
Choi and co-workers[24] prepared mechanical crack-based ultra-
DOI: 10.1002/adfm.201601995 sensitive strain sensors, which were highly sensitive to strain

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and vibration with a gauge factor (GF) of 2000 in the 0–2%
strain range, benefiting from the disconnection–reconnection
process of cracks. Zhu and co-workers[26] developed highly
sensitive strain sensors with channel cracks by structural engi-
neering of gold thin films. Additionally, Shi and co-workers[28]
prepared strain sensors with microsized cracks based on gra-
phene coated human hairs. However, the electrical conductance
of the crack junctions experiences a sudden jump from a finite
value when the crack junctions are in contact to zero when
they disconnect. Most sensors based on pure crack mechanism
exhibit a limited detection range due to the easy breakage of
conductive pathways, inhibiting their application in large defor-
mation detections. Furthermore, pressure sensors based on
crack mechanism are rarely explored by far.
In this work, we demonstrate a very simple and cost-efficient
strategy for fabricating flexible, highly sensitive, and versatile
pressure-sensing platform based on commercial carbon black
(CB) and PU sponges. CB is uniformly coated on PU sponges
via natural polymer-mediated water-based layer-by-layer (LBL)
assembly, forming conductive CB@PU sponges. Using these
CB@PU sponges, a wide range of deformations from 0.2% to
60% strain (corresponding 91 Pa–16.4 kPa) can be monitored
in real time. The high sensitivity and versatility of the CB@PU
sponges in pressure sensing are based on a synergistic effect
of two mechanisms: variation of microcrack junctions in CB
layer and contact-separation of CB@PU conductive backbones.
Moreover, this CB@PU pressure-sensing platform exhibits
excellent flexibility, fast response time (<20 ms), as well as good
reproducibility over 50 000 cycles. We also confirm the versatile
capabilities of this pressure-sensing platform in speech recog-
nition, health monitoring (pulse, breathing), human activities
detection (swallowing, coughing, joint bending), and artificial
electronic skin. The comprehensive performance of our sen-
sors is comparable to that of the recently reported pressure
sensors,[30–38] simultaneously offering advantages of simplicity,
low-cost, large-area compliance, environmentally friendly fabri-
cation process as well as versatility in monitoring wide range
of pressure stimuli. To the best of our knowledge, this is the
first demonstration that highly sensitive and versatile pres-
sure sensors can be fabricated using such cheap raw materials
and simple processes, which opens up new opportunities for
the widespread fabrication and application of pressure-sensing
devices.
2. Results and Discussion
2.1. Preparation of CB@PU Sponges
CB is an abundant material with desirable conductivity and
cost advantage over other conductive fillers. It has been widely
used in conductive polymer composites. However, the poor
dispersibility of CB in water makes it infeasible to form uni-
form and controllable CB conductive layers through water-
based LBL assembly (Figure S1, Supporting Information). In
this study, we demonstrated that CB could be well stabilized
by appropriate environmentally friendly natural polymers, i.e.,
cellulose nanocrystal (CNC) and chitosan (CS). Thus, we could
obtain stable negatively charged CB− (CB@CNC) and positively
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charged CB+ (CB@CS) suspensions (Figure S1, discussed in
FULL PAPER
Supporting Information). The oppositely charged and well sus-
pended CB makes it feasible to form controllable conductive
layers on various matrices via water-based LBL assembly.
Figure 1a shows the schematic fabrication procedure of
CB@PU sponges via natural polymer-mediated water-based
LBL assembly. A cleaned PU sponge (Figure 1b) was alternately
dipped into oppositely charged CB suspensions, allowing elec-
trostatic deposition of CB on the surface of PU backbones.
Compared to the original PU sponge, CB@PU sponge turned
black (Figure 1c). Scanning electron microscopy (SEM) images
(Figure 1d,e) show that a PU sponge has a 3D porous structure.
The surface of PU backbones is very smooth (Figure 1f). After
electrostatic deposition of CB on a PU sponge, the surface of
CB@PU backbones became rugged as shown in Figure 1g,h.
CB particles could be observed clearly in Figure 1i, indicating
that a CB layer was deposited on the surface of PU backbones.
In addition, the electrical conductivity and elastic modulus of
CB@PU sponges are found to increase with more LBL deposi-
tion cycles of CB (Figure S2b and Table S1, Supporting Infor-
mation), resulting from the increasing CB mass on PU sponges
(Figure S2a, Supporting Information). All the results demon-
strate that a conductive CB layer has been successfully coated
on a PU sponge via water-based LBL assembly. It is worth
noting that the fabricating cost of CB@PU sponges is very low
as given in Table S2 in the Supporting Information. Further-
more, the resultant CB@PU sponges exhibited excellent flex-
ibility during bending, compressing, and twisting as shown in
Figure 1j–l. The desirable flexibility and low cost of CB@PU
sponges make this material qualified for manufacturing flexible
pressure sensors on large scale.
2.2. Pressure-Sensing Mechanism
Spiders can detect very small vibrations in their surround-
ings, benefiting from their crack-shaped slit organs near the
leg joints between metatarsus and tarsus bones, as shown in
Figure 2a.[20,24] Small external force variation causes deforma-
tion of the slit, which can be perceived by the neurons system
under the slit. Inspired by this ability, we selected the rigid and
spherical CB nanoparticles as a conductive filler to form conduc-
tive layers on PU sponge, rather than fillers with high aspect
ratio (such as carbon nanotube, graphene, or metal nanowires,
etc.) which could result in entangling or stacking with each
other. When applying a mechanical compression to the CB@
PU sponges, bending of the backbone caused tension on the CB
layer. Hence, permanent mechanical microcracks could be easily
generated in the CB layers (Figure 2c,d). When releasing the
compression, microcracks closed and formed crack junctions.
In the subsequent pressure-sensing process, reversible discon-
nection–reconnection of the mechanical microcrack junctions
(as illustrated in Figure 2b) caused breakage-recovery of the
local conductive pathways, leading to corresponding variations
in electrical conductance. Specifically, a finite value of electrical
conductance could be obtained when the edges of the microc-
racks were in contact. Once the edges disconnected, the electrical
conductance experienced a sudden drop, exhibiting responsive
behaviors to strain stimuli. This mechanical microcrack design
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Figure 1. a) Schematic diagram for preparation of CB@PU sponges. b) Photographs of a neat PU sponge and (c) CB@PU sponge. d–f) SEM images
of a neat PU sponge and (g–i) CB@PU sponge, magnification: 50× (d,g), 200× (e,h), and 20 000× (f,i). j–l) Photographs showing the excellent flexibility
of CB@PU sponges during bending, compressing, and twisting.

that mimics slit geometry of spiders is expected to attain high
sensitivity of the sensors, thus to detect ultrasmall deformations.
However, with further increased compressive strain, the dis-
connected microcrack joints failed to give a response to larger
strains. Hence, versatile pressure sensors with desired sensing
capability in broad pressure range are desirable.
In addition, the CB@PU sponges possess combinational
compressibility and electronic conductivity, which makes the
sponges capable of detecting large deformations as well. Spe-
cifically, compressive deformations cause contact-separation of
CB@PU conductive backbones under high strains (Figure 2e,f),
resulting in conductance modulation of CB@PU sponges

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Figure 2. a) Sketch of the crack-shaped slit organs near the leg joints of spider. b) Schematic variations of mechanical microcrack junctions in the
CB layer of CB@PU sponges under small deformation. Small strains caused disconnection–reconnection of the mechanical microcrack junctions.
SEM images of the microcrack junctions on a CB@PU sponge after compressing pretreatment, magnification: c) 2000× and d) 4000×. Schematic
illustrations for large-scale compressive deformation of CB@PU sponges. e,f) High strains mediated the contact area between CB@PU conductive
backbones. g) SEM images of an uncompressed and (h) compressed CB@PU sponge, magnification: 100×. i) Schematic evolutions of the conductive
pathways in a CB@PU sponge during continuous compressive deformation. Disconnection of microcrack junctions in the CB layer occurred upon small
deformations and caused breakage of local conductive pathways (middle). CB@PU backbones contacted with each other upon large deformations,
leading to formation of more conductive pathways in the CB layer (right).

(higher strain leading to larger contact area between CB@PU
conductive backbones). Figure 2g presents an SEM image of a
CB@PU sponge before loading compressive strain. The orig-
inal CB@PU sponge owned 3D, cellular-like networks with
individual backbones. While the microcellulars deformed and
even distorted under high compressive strain (60%) (Figure 2h).
It is noticed that some CB@PU backbones contacted with each
other (Figure 2h inset and Figure S3, Supporting Information),
leading to an increase of contact area between the conductive
backbones. The variation of the contact area between CB@PU
backbones made CB@PU sponges capable of detecting large
compressive strains.
As illustrated in Figure 2i, when increasing pressure is
applied upon CB@PU sponges, microcrack junctions in the
CB layer disconnect first. Notably, these microcrack junctions
are distributed at the weakest positions of the conductive back-
bones as shown in Figure S4 (Supporting Information). Thus,
the breakage of local conductive pathways results in an elec-
trical conductance drop of the whole CB@PU sponges (dis-
cussed in Supporting Information). As the compressive strain
gradually increases, the crack-gap and crack-density extends
correspondingly (Figure S5, Supporting Information), which
further decreases the conductivity of the CB layers (Figure 2i
middle). When the applied strain reaches a certain value, how-
ever, some CB@PU backbones contact each other. This pro-
motes the formation of more conductive pathways in the CB
layer (Figure 2i right), leading to a rise in electrical conductance
of the CB@PU sponges. These two mechanisms mentioned
above work simultaneously, and exhibit a synergistic effect
on the pressure-sensing behavior of CB@PU sponges, which
endows CB@PU sponges with a high sensitivity as well as the
versatility to detect wide range of deformations.
2.3. Piezoresistive Properties of CB@PU Sponges
The electrical characteristics of CB@PU sponges under pres-
sure are presented in Figure 3. Opposite sides of the sam-
ples were coated with conductive silver paste (Figure S6a,
Supporting Information) to eliminate the contact resistance,
and to obtain stable signal output. Upon a constant voltage,
electrical current of CB@PU sponges was recorded with the

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Figure 3. a) Responsive current curve of a CB@PU sponge versus compressive strain along with the corresponding GF variation (inset). b) Relative
resistance change (ΔR/R0) versus progressively increasing pressure. Repeatedly compressing tests of a CB@PU sponge at (c) small and (d) large
strains. e) Instant response of CB@PU sponges, which shows a response time of 20 ms. f) Reproducibility test of a CB@PU sponge for 50 000 cycles
at 40% strain.

variation of pressure. The pressure was applied at normal direc-
tions, causing changes in thickness, i.e., compressive strains
(Figure S6b, Supporting Information). The responsive behaviors
of CB@PU sponges with different LBL cycles were investigated
and discussed in Supporting Information (Figure S7 and S8). A
sample of CB@PU sponge with 15 LBL cycles, which exhibited
desirable responses to compressive strains, was employed for
the following tests unless otherwise specified.
Figure 3a shows a typical responsive current curve of CB@
PU sponges with progressively increasing strain. It can be
seen that the current signal experienced a rapid decline in the
strain range of 0–9% (A stage), revealing a decrease in elec-
trical conductance. This could be attributed to the disconnec-
tion of mechanical microcrack junctions in CB layers, followed
by the increasing of crack-gap and crack-density under higher
strains (Figure S5, Supporting Information). As the applied
strain increased progressively (9–52%, B stage), however, the
current values increased slowly. This is due to the increased
contact between CB@PU conductive backbones, which coun-
teracted the effect of microcracks. It became a dominant factor
for the resistance change (Figure 2h,i). When the applied strain
reached 52% (C stage), the current began to rise quickly. In
this stage, increasing contact area between CB@PU backbones
played a decisive role for the resistance change. GF, which
is defined as the ratio of relative resistance change (ΔR/R0)
versus strain, was calculated to assess the sensitivity of CB@
PU sponges to applied strains. As shown in Figure 3a inset,
the GF in A stage (<9% strain) was calculated to be 2.2. In B
stage (9–52% strain), the average GF value dropped to −0.38.
However, in C stage (52–60% strain), the GF reached −3.1.
These data reveal that in low and high strain regions, CB@PU
sponges exhibit higher sensitivity to compressive strain than
that in middle strain region.
In addition, the sensitivity of CB@PU sponges to applied
pressure was also investigated. The plot of ΔR/R0 versus applied
pressure is shown in Figure 3b. It is noticed that the pres-
sure responsive behaviors of CB@PU sponges could also be
divided into three regions: positive A region and negative B and
C region. In A region, ΔR/R0 shows a linear increase against
progressively increasing pressure, exhibiting a positive sensi-
tivity slope of 0.068 kPa−1, which is comparable to that of some
recently reported sensors.[4,17,30–32] In this region, mechanical
microcrack-induced resistance increase played a decisive role.
However, when the applied pressure exceeded 2.3 kPa, contacts
between CB@PU conductive backbones became a dominant
factor, and resulted in a negative sensitivity slope of 0.023 kPa−1
in B region and 0.036 kPa−1 in C region.
The responsive behaviors of CB@PU sponges to small
repeated compressive strain variations (Figure S9, Supporting
Information) were recorded. As shown in Figure 3c, stable and
continuous current responses could be observed. Notably, a
compressive strain as low as 0.2%, corresponding a pressure
of 91 Pa, could be detected (Figure 3c). This minimum detect-
able limit is lower than that of some recently reported sen-
sors.[30,32–34] As compressive strain increases to 5%, the inten-
sity of signals becomes higher. These responses of CB@PU
sensors to small compressive strains might enable us to discern
tiny motions, such as airflow, pulse, speech, and so on.
At the large repeated strain region, a series of character-
istic and noise-free signal outputs were obtained (Figure 3d).
The intensity as well as the shape of these signal peaks varied
with each other at different strain values. The higher the strain

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reached, the sharper the peaks became. These distinguishing
responsive signals in large strain region make the CB@PU
sponges capable of detecting and differentiating large-scale
human movements, such as joint bending and breathing.
Figure 3e shows that the instant response of our CB@PU
sponges exhibited a fast response time of <20 ms, which is
faster than those selected from the world’s best sensors.[14,35–38]
The fast response time of this sensor ensures a stable response
to compressive strains as discussed in Supporting Information
(Figure S10), and could realize the synchronic monitoring of
human motions. The reproducibility of the CB@PU sponges
was also evaluated. As given in Figure 3f, during 50 000
loading–unloading cyclic tests at 40% strain, the responsive
signal output was nearly invariable, except for a current shift
due to the slight decrease in conductivity (Figure S11, Sup-
porting Information). The excellent reproducibility of this
sensor can be ascribed to the desirable compression-resilience
properties of the CB@PU sponges (Figure S12), as discussed
in Supporting Information. Additionally, the repeatability of
the samples was assessed as well (see Figure S13, Supporting
Information), which reveals that different CB@PU sponges
have similar response behaviors to pressure.
2.4. Small-Scale Motion Monitoring
We evaluated the capabilities of this flexible and sensitive CB@
PU sponges in monitoring small-scale human activities. First,
a CB@PU sensor was attached to the neck to noninvasively
detect the muscle motions near the throat (Figure 4a). When
the tester pronounced different words (such as bee, dog, snake,
and mosquito), current changes of the sensor were recorded.
As shown in Figure 4b and Movie S1 and S2 in the Sup-
porting Information, nearly same current patterns were pro-
duced when the word was repeated, indicating the stability of
this sensor. Additionally, the current patterns varied when dif-
ferent words were pronounced, since each word resulted in dif-
ferent motions of the vocal muscle. The significant differences
between these current signals reveal a good possibility for this
sensor to act as voice recognition devices. Besides, when the
tester swallowed saliva, the motions around the throat resulted
in more distinct current patterns (Figure 4c). Coughing and
chewing could also give characteristic signal patterns as shown
in Figure 4d,e. These characteristic current signals enable us to
differentiate the motions near the throat, which makes it pos-
sible for this sensor to monitor and distinguish human’s physi-
ological activities.
Then, the CB@PU pressure sensor was attached to the wrist
to monitor the blood pulse of human radial artery in real-time
(Figure 4f). As can be seen clearly in Figure 4g and Movie S3
in the Supporting Information, the wrist pulse could be read
out accurately from the time-dependent current signals with a
periodicity of 84 beats per minute. The measured single wrist
pulse could be divided into two distinguishable peaks: systolic
peak and diastolic peak, marked as P1 and P2, respectively
(Figure 4h). Based on these data, the radial augmentation index
(P2/P1), which is an important value for characterizing arterial
stiffness, can be calculated. From the waveforms measured
by the CB@PU pressure sensor, an average P1/P2 value was
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estimated to be 0.52, which is in accordance with the literature
data[39] for a healthy 174 cm tall, 25 year old male. The transit
time (ΔTDVP), which is defined as the time delay between sys-
tolic peak and diastolic peak,[16,40] could also be obtained from
Figure 4h. As a contrast test, once the CB@PU sensor left the
wrist, no current variations could be observed (Figure S14, Sup-
porting Information). These results confirm that our CB@PU
pressure sensor has the capacity to identify sophisticated dif-
ferences in blood pulses, exhibiting its potential in diagnostic
applications.
Figure 4i shows the detection of airflows generated by
blowing air from the mouth. At first, the tester blow air gently
towards a CB@PU sponge (10 mm × 10 mm). Responsive
decline peaks of current could be observed, resulting from
the weak air movement. With the airflow became heavier, the
intensity of the signal peaks increased correspondingly. This
ability of CB@PU sensors can be adapted to detect a variety of
non-contact actions in certain potential applications, such as
turbulent flow detection, acoustic transduction, and so on.
To determine the detection limit of the CB@PU sensors, we
loaded a very small grain of rice (27 mg) on a CB@PU sponge
(4 mm × 4 mm), giving a pressure of 17 Pa on the sensor
(Figure 4j, inset). Upon loading the rice, a small decline peak
of current was detected (Figure 4j), which was ascribed to the
weak impact of the rice on the sensor. After that, the current
experienced a recovery process, but still maintained at a lower
state when compared to the original value. The small deteriora-
tion of current resulted from the small pressure (17 Pa) caused
by the rice grain. These data demonstrate the ultrahigh sensi-
tivity of the CB@PU sponge sensor.
2.5. Large-Scale Motion Monitoring
Apart from tiny motion detections, the CB@PU sponge pres-
sure sensors are qualified for large-scale movement monitoring,
benefiting from its high compressibility and piezoresistive per-
formance under large compressive strains. Figure 5a shows
the fabrication of a waistband-based breath monitoring device.
A piece of CB@PU sponge, coated with silver paste on oppo-
site sides, was attached onto the flank of a rigid waistband. The
CB@PU sponge equipped waistband was then girded on the
waist of a tester. During breathing in, the CB@PU sponge was
compressed, accompanied with a decrease in current value of
the substrate (as illustrated in Figure S15, Supporting Informa-
tion). During breathing out, the compressed CB@PU sponge
relaxed and returned to its original state, resulting in recovery
of the current signal. The repeated compressing-releasing pro-
cesses gave typical current variations as shown in Figure 5b.
The respiratory rate with a periodicity of 59 times per minute
could be obtained from the recorded current signal. This con-
firms the ability of this sensor in human breath monitoring.
In order to further demonstrate the capabilities of this flex-
ible sensor in large strain detecting, a CB@PU sponge was
mounted on the joint of index finger with medical adhesive
tapes (Figure S16, Supporting Information). The tester was
conducted to perform finger bending-release sequences. We
checked the currents signals of the CB@PU sensor at six dif-
ferent bending-release motions of the finger, which are labeled
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Figure 4. a) Photograph of CB@PU pressure sensor attached to the throat to monitor human’s physiological activities. b) Recorded current signal
versus time during pronouncing, c) saliva swallowing, d) coughing, and e) chewing, respectively. f) Photograph of CB@PU sensor attached to the wrist
to measure the pulse. g) Original signal of current curves for wrist pulse monitoring. h) Zoomed waveform extracted from the original signal, showing
some important features that are essential for health monitoring. i) Current response of CB@PU sensor to the air movements generated by blowing
from mouth. j) Current change of CB@PU sensor upon loading a grain of rice with a weight of 27 mg.

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Figure 5. a) Photographs showing a human breath sensor fabricated by attaching a CB@PU sponge onto a waistband. b) Recorded current–time
curve during human breath monitoring. c) Current signal of the sensor device that was fixed on an index finger at six different bending- release finger
motions. The bottom insets labeled as I, II, III, IV, V, and VI demonstrate the four finger motion states, and the upper insets labeled as I, II, and
III give the magnified signals of motion—I, II, and III. d) The excellent repeatability of this sensor in finger bending test. e) Photographs of arm bending
monitoring by using a CB@PU sponge and (f) the corresponding current signals.

as state I, II, III, IV, V, and VI in the bottom insets in Figure 5c.
It can be observed that the sensor gave different responsive
signals to different motions of the finger (Movie S4, Sup-
porting Information). In detail, the current signal showed a
sharp decrease peak upon small-scale bending release of the
finger (motion-I). Motion-II also caused a decrease peak of the
current signal, while a small increase peak could be observed
in the peak valley. However, the current value showed sharp
increase peaks upon large-scale motions (motion-III, motion-
IV, motion-V, and motion-VI). The larger the motion range
was, the higher the peak intensity reached. These could be
attributed to that: small-scale motions caused mild compres-
sion of the sensor and resulted in disconnection of mechanical
microcrack junctions in CB layers (corresponding to A stage in
Figure 3a); while, large-scale motions caused strong compres-
sion of the sensor and led to increase of contact area between
the conductive backbones (corresponding to B and C stages in
Figure 3a). These results confirm the satisfactory capability of
our CB@PU sensor to distinguish different-scale motions of
the finger.
It is noticed that the current responses exhibit outstanding
stability and reproducibility in finger bending-release motions
(Figure 5d), indicating the good reliability of this sensor. Fur-
thermore, when a CB@PU sponge was attached to the outside
of the elbow, distinct and repeatable current signals could also
be recorded during the elbow bending (Figure 5e,f). These
results demonstrate the capabilities of the CB@PU sponge
sensors in large-scale movement monitoring, which might be

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adapted to athlete training data acquisition systems, instrument
control for physically challenged patients, and so on.
2.6. Electronic Skin
The soft and flexible CB@PU sponges feel like human skin
because of its elasticity. Along with its low cost as well as fea-
sibility in large-area production, the CB@PU sponges have
great potential in manufacturing pressure-sensitive artificial
electronic skin. As a typical demonstration, we integrated a
piece of CB@PU sponge (65 mm × 65 mm) into an artificial
electronic skin with 6 × 6 pixel arrays, as shown in Figure 6a.
The schematic model of this CB@PU artificial electronic skin
is given in Figure 6b. Small pieces of silver paste, which acted
as the sensing pixel elements, were attached onto both sides
of the CB@PU sponge and connected by bent copper wires.
Upon applying pressure on the electronic skin, the resistive
variation of each pixel was measured and the color contrast
mapped with the local pressure distribution was plotted. As
shown in Figure 6c, when a pen was pressed on the electronic
skin, the resistive variation depended on the specific location
of the applied pressure. The spatial pressure distribution was
consistent with the location of the pen (see Figure 6d). Next,
an index finger was pressed on another position of the artificial
electronic skin (Figure 6e). It was noticed that the color contrast
mapping could reveal the distribution of pressure as well as the
shape of the finger pad. These results demonstrate the potential

Figure 6. a) Photograph showing a CB@PU based artificial skin with 6 × 6 pixels, and (b) the model of the CB@PU based artificial skin for measuring
spatial distribution of the applied pressure. Photographs of a (c) pen and (e) finger pressed on the surface of as-prepared artificial skin, and (d,f) cor-
responding maps of the estimated pressure profile over a 2D area based on the change in resistance.

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application of our CB@PU sponges as artificial electronic skins
that can simultaneously detect the location and shape of an
object. In the future, more pixels could be integrated into the
CB@PU based electronic skin by using an advanced photoli-
thography technique[41,42] for higher resolution of the CB@PU
electronic skin.
3. Conclusions
In summary, we demonstrated a very simple and low-cost
strategy to fabricate a flexible, highly sensitive, and versatile
pressure-sensing platform based on CB and PU sponges for
human–machine interfacing applications. The combination of
the microcrack junction sensing mechanism inspired by the
spider sensory system and the compressive contact of CB@PU
conductive backbones endowed CB@PU sponges with high sen-
sitivity and capabilities of monitoring ultrasmall as well as large
motions. Notably, the CB@PU based pressure sensors exhibited
excellent flexibility, fast response time of <20 ms as well as good
reproducibility over 50 000 cycles. Various human activities
(such as pronouncing, coughing, swallowing, pulse, breathing,
joint bending, etc.) could be monitored in real-time using this
highly sensitive and versatile pressure-sensing platform. This
pressure-sensing platform is comparable in comprehensive
performance with recently reported devices, simultaneously
possessing advantages of low-cost, simplicity, and versatility of
detecting various human activities. We believe that this simple
but efficient strategy for manufacturing pressure-sensitive mate-
rials will make a step further towards low-cost personal elec-
tronics and biomedical devices in the near future.
4. Experimental Section
Preparation of CB@PU Sponges: CB@PU sponges were fabricated via
LBL assembly by alternately dipping PU sponges into oppositely charged
CB suspensions. PU sponges were cut from commercial cleaning
sponges (3M company). CB (BP 2000) was purchased from Cabot
Chem., USA. CNC was prepared by controlled acid hydrolysis of cotton
fibers according to our previous studies.[43,44] For preparation of CNC-
stabilized CB− suspension, 0.2448 g CB was added into 800 mL CNC
(0.613 mg mL−1) suspension. The mixture was sonicated for 30 min
(1200 W), yielding well-suspended and negatively charged CB@CNC
suspension. Positively charged CS stabilized CB+ suspension was
prepared as mentioned above except for the employment of CS. Then, a
cleaned PU sponge was dipped into CB+ suspension, forming positively
charged CB+@PU sponge. The excess CB+ suspension was squeezed
out. Subsequently, the CB+@PU sponge was dipped into a oppositely
charged CB− suspension, and squeezed out the excess CB− suspension.
This process was repeated for x times, and the corresponding sample
was labeled as LBLx. During this process, the CB@PU sponge was dried
after every five LBL cycles. Finally, the obtained CB@PU sponge was
dried at 80 °C for 6 h to remove the moisture.
Pressure Sensor Fabrication: Opposite sides of a CB@PU sponge were
coated with conductive silver paste to eliminate the contact resistance,
and to obtain steady signal output. Two copper wires were embedded in
the conductive silver paste and connected to an analyzer to the record
the current variation under corresponding compression. During small
and large motion monitoring, the CB@PU sponge-based pressure
sensor was attached to the testing position by using medical adhesive
tapes. The degree of tightness was adjusted until steady current signals
were obtained. A thin layer of PDMS (Dow Corning Sylgard 184; ratio of
Adv. Funct. Mater. 2016, 26, 6246–6256 © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
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FULL PAPER
base to crosslinker, 15:1 by mass) was coated on the surface of the silver
paste to minimize the effect of the conductivity of human skin on the
performance of the sensor.
Fabrication of Pressure-Sensitive Skin: A piece of CB@PU sponge with a
size of 65 mm × 65 mm × 5 mm was used for fabrication of the artificial
electronic skin with 6 × 6 pixels. Small silver paste pieces were pasted
onto the upper surface of CB@PU sponge as electrodes to form 6 pixel
× 6 pixel arrays. The small silver paste pieces on the column selection
were connected by bent copper wires. The silver paste pieces on the row
selection were also connected by bent copper wires. The bottom surface
of the CB@PU sponge was pasted with silver paste pieces as same as
the upper surface. Finally, both sides of the CB@PU sponge were coated
with a thin layer of PDMS to form insulating layers.
Characterization: Zeta potential (ζ potential) of CB, CB@CNC, and
CB@CS were measured using a Zetasizer nano-ZS (Malvern, UK)
instrument. SEM was performed on a microscope (JEOL JSM-5900LV,
Japan). The piezoresistive properties of all samples were measured in
real-time by a two-point measurement with a Keithley 2601B source
meter (USA) and copper clamps. Compression tests were conducted on
a versatile testing machine (Instron-5560, USA) at room temperature.
Supporting Information
Supporting Information is available from the Wiley Online Library or
from the author.
Acknowledgements
The authors thank the National Science Foundation of China (51203105
and 51473100) and State Key Laboratory of Polymer Materials
Engineering (Grant No. sklpme2015-3-04) for financial support.
Received: April 21, 2016
Revised: May 26, 2016
Published online: June 29, 2016
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