Biosensors and Bioelectronics 123 (2019) 167–177

Contents lists available at ScienceDirect

Biosensors and Bioelectronics

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

Recent developments in bio-monitoring via advanced polymer T

nanocomposite-based wearable strain sensors
⁎ ⁎⁎
Yang Lua, Manik Chandra Biswasb, Zhanhu Guoc,d, Ju-Won Jeonb,e, , Evan K. Wujcika,
a
Materials Engineering and Nanosensor [MEAN] Laboratory, Department of Chemical and Biological Engineering, The University of Alabama, P.O. Box 870203,
Tuscaloosa, AL 35487, USA
b
Jeon Research Group, Department of Chemical and Biological Engineering, The University of Alabama, P.O. Box 870203, Tuscaloosa, AL 35487, USA
c
Integrated Composites Laboratory (ICL), Department of Chemical & Biomolecular Engineering, University of Tennessee, Knoxville, TN 37996, USA
d
College of Chemical and Environmental Engineering, Shandong University of Science and Technology, Qingdao, Shandong 266590, China
e
Department of Applied Chemistry, Kookmin University, Seoul, Republic of Korea

A R T I C LE I N FO A B S T R A C T

Keywords: Recent years, an explosive growth of wearable technology has been witnessed. A highly stretchable and sensitive
Wearable wearable strain sensor which can monitor motions is in great demand in various fields such as healthcare,
Strain robotic systems, prosthetics, visual realities, professional sports, entertainments, etc. An ideal strain sensor
Sensor should be highly stretchable, sensitive, and robust enough for long-term use without degradation in perfor-
Bio-monitoring
mance. This review focuses on recent advances in polymer nanocomposite based wearable strain sensors. With
Polymer
the merits of highly stretchable polymeric matrix and excellent electrical conductivity of nanomaterials, polymer
Nanocomposite
nanocomposite based strain sensors are successfully developed with superior performance. Unlike conventional
strain gauge, new sensing mechanisms include disconnection, crack propagation, and tunneling effects leading to
drastically resistance change play an important role. A rational choice of materials selection and structure design
are required to achieve high sensitivity and stretchability. Lastly, prospects and challenges are discussed for
future polymer nanocomposite based wearable strain sensor and their potential applications.

1. Introduction response to motions of wearer (Lu et al., 2016; Pantelopoulos and

Bourbakis, 2010; Rogers et al., 2010; Salvatore and Tröster, 2015).
With the recent advances in modern wearable bioelectronic devices Strain sensing is one of the most important applications of wearable
and nanotechnology, great effort have been made in polymer nano- sensor devices. Though many different types of flexible strain sensors
composite based wearable strain sensors for healthcare and medical have been developed or reported, including fiber Bragg grating (FBG),
diagnosis, robotic systems, prosthetics, visual realities, professional raman shift, liquid metals, triboelectricity and piezoelectricity based
sports, entertainments, among others (Rogers et al., 2010). Wearable strain sensors (Chossat et al., 2013; Gullapalli et al., 2010). However,
devices can be attached onto clothes, garments or directly worn on the the complexity of fabrication, poor dynamic performance, low resolu-
human skin by adhesive tapes or elastic straps for monitoring physical, tion and requirement of advanced measurement devices have con-
biochemical signals and motions (Park et al., 2015b; Sazonov and strained their applications. In contrast, resistive-type and capacitive-
Neuman, 2014). Mechanical flexibility is extremely important for type strain sensors are more practical and popular due to their low cost,
wearable devices to minimize the discomfort of worn or attached ease of fabrication and integration, easy read-out unit, high flexibility
electronics, in short, it should behave like the human skin (Sazonov and and high strechability (Cai et al., 2013; Larimi et al., 2018). They re-
Neuman, 2014; Someya et al., 2016). Due to the soft, complaint nature spond to the mechanical deformations by the change of resistance or
of human tissues and the natural bending or rotational motion asso- capacitance. Conventional strain sensors are inexpensive; however,
ciated by joints, both the structure and materials should be soft and they typically have very limited stretchability (< 5%) and bulky com-
mechanically robust enough to bend, stretch, press, and twist in ponents (Amjadi et al., 2014; Monty et al., 2013; Wujcik et al., 2013).

⁎
Corresponding author at: Jeon Research Group, Department of Chemical and Biological Engineering, The University of Alabama, P.O. Box 870203, Tuscaloosa,
AL 35487, USA.
⁎⁎
Corresponding author at: Materials Engineering and Nanosensor [MEAN] Laboratory, Department of Chemical and Biological Engineering, The University of
Alabama, P.O. Box 870203, Tuscaloosa, AL 35487, USA.
E-mail addresses: [email protected] (J.-W. Jeon), [email protected] (E.K. Wujcik).

https://doi.org/10.1016/j.bios.2018.08.037
Received 29 June 2018; Received in revised form 15 August 2018; Accepted 16 August 2018
Available online 22 August 2018
0956-5663/ © 2018 Elsevier B.V. All rights reserved.
Y. Lu et al. Biosensors and Bioelectronics 123 (2019) 167–177

Table 1
Mechanical properties of some common materials (Someya et al., 2016).
Material Young's Modulus Elongation at Break

Silicon 130 GPa 1%

Bone ~ 20 GPa 1%
Plastics 1 GPa 5%
Elastomer 0.01–10 MPa 50–4000%
Gel 1–1000 kPa 10–2000%

The demand for high performance wearable strain sensor has drama-
tically increased with the advances of science and technology. Devel- Fig. 1. Illustration of strain in materials.
oping novel stretchable sensor which could sustain a high strain with
the preservation of conductive pathways is a key point (Zhao et al., piezoresistive effects. For stretchable resistive-type strain sensors, the
2017a). Conventional semiconductors including silicon, and metal change of resistance are mainly due to disconnection of conductive
oxide films possess an intrinsic brittle and rigid nature, which limits fillers, crack propagation at large strain and tunneling effect between
their applications in wearable devices requiring intimate integration closely positioned conductive fillers. Strain is defined as the ratio of the
with curvilinear surfaces (clothes, human skin, etc.) and large de- change in length of a material to the original length, as shown in Fig. 1.
formation (bending, stretching, twisting, etc.) (Blasdel et al., 2015; Yao Strain can be positive when material is elongated by tensile stress, while
and Zhu, 2015). Improved conformability and bendability can be it can also be negative when compressed. There are four types of
achieved by using ultrathin films of silicon or metal oxide semi- strains: axial, bending, shear, and torsional, in which axial and bending
conductors. However, reducing the thickness does not change the strains are most common.
Young's modulus and stretchability (low elongation at break) of the
silicon film which make it impractical for strain sensors (Table 1). To
2.1. Geometric effect
address this challenge, there are generally two main strategies in de-
signing stretchable strain sensors: "structures that stretch" and "mate-
Geometric effect is the main mechanism for capacitive-type strain
rials that stretch" (Khang et al., 2006). A polymer nanocomposite based
gauges. This effect also plays a role in highly stretchable resistive-type
strain sensor typically has two main components, one is the conductive
strain sensors but is believed not as crucial as other mechanisms. When
network (act as the sensing element) which can provide conductive
the materials are stretched, they tend to contract in transverse direc-
pathways to produce signal, and the other component is an elastomeric
tions to the stretched direction. Similarly, when they are compressed,
polymer to provide flexibility, stretchability and protection for con-
they tend to expand in transverse directions following Poisson's ratio of
ductive network (Zhao et al., 2017a). As for the operation of stretchable
ν. For highly stretchable elastomers, the Poisson's ratio value is nearly
strain sensors, it should be easy to establish as they are no-invasive
0.5. From Ohm's Law, the resistance of a conductor is given by R = ρL/
wearables at current stage of applications. Due to the fact that signals
A, where ρ is the electrical resistivity, L is length and A is the cross
are produced by the physical strain changes of underlying subjects such
section area of the conductor. When the conductor is at a stretched
as skin, clothing, etc. the strain sensor does not require intimate direct
state, L increases while A decreases, which makes an increment in
contact with skin as long as the adhesion is strong enough to con-
measured resistance (Hempel et al., 2012). However, for resistive-type
tinuously experience the same degrees of strain for accurate mon-
strain sensor, the large degree of deformation takes place at elastomer
itoring. The encapsulation of strain sensor using an appropriate bio-
matrix phase, while conductive fillers slip out each other or conductive
compatible, stretchable barrier polymer (such as silicone based
network sustains a structure deformation. The geometric change of
elastomers: poly(dimethylsiloxane) (PDMS), Ecoflex, etc.) or adhere
conductive materials is extremely limited. For capacitive-type strain
strain sensor onto skin tight clothes can help prevent the direct inter-
sensor, it can be treated as a simple parallel-plate capacitor where the
action with body fluids and external environment which may interfere
overlapped length is l0, width is w0, and thickness of dielectric layer is
the receiving resistive or capacitive signals. The majority of reported
d0 (Yao and Zhu, 2014). The initial capacitance is given by Eq. (1):
elastomeric polymers (See Section 4.1 for details) as matrix have a wide
useful working conditions as they are chemically inert, not light sen- l 0 w0
C0 = ε0 εr
sitive, waterproof in temperature ranges between − 45 to 200 °C. Note d0 (1)
that some types of conductive fillers might limit the useful working
Where ε0 and εr are the electric and dielectric constant of dielectric
conditions.
layer, respectively. At strain ε, the length l are stretched to (1 + ε) l0,
This review focuses on the background and recent advances of
while width and thickness are contracted to (1- νelectrode ε) w0 and (1-
polymer nanocomposite based wearable strain sensors in four sections:
νdielectric ε) d0, respectively, the capacitance will be:
First, strain sensing mechanisms are introduced. Second, performance
metrics such as stretchability, gauge factor (GF), linearity, hysteresis (1+ε ) l0 (1− νelectrode ε ) w0
and features including self-healing, transparancy, etc. of recent reported C = ε0 εr
(1− νdielectric ε ) d 0 (2)
strain sensors are discussed. Third, the choice of materials selection
including elastomeric substrate and conductive nanomaterials are re- For most stretchable strain sensors, the Poisson's ratios of electrode
viewed. Finally, we point out some challenges that need to be addressed and dielectric layers are close to 0.5. The capacitance at stretched state
to make current stretchable strain sensors more practical in future ap- is close to C = (1 + ε ) C0 , giving capacitive-type strain sensor an ex-
plications. cellent linearity (Yao and Zhu, 2014). However, some studies reported
that when strain is too high, the linear relationship will not be valid
2. Sensing mechanisms anymore (Amjadi et al., 2016).

Because polymer nanocomposite based strain sensors have multi- 2.2. Piezoresistive effect
phase, designed structures and conductive networks constructed by
nanomaterials, their sensing mechanisms are different from conven- The piezoresistive effect is a change in electrical resistivity of ma-
tional strain gauges which solely dependent on geometric and intrinsic terials when a mechanical strain is applied. For metals and

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semiconductors, the change of resistance at strain ε can be written as:

∆R ∆ρ
= (1 + 2ν) ε +
R ρ (3)
∆ρ
Where (1 + 2ν) ε is the geometric effect, and is the fractional change
ρ
in resistivity (intrinsic piezoresistive effect) (Barlian et al., 2009). Pie-
zoresistive effect for metal is as small as around 0.3. However, for
semiconductors such as silicon and germanium under certain direc-
tions, the change in resistivity can be 50–100 times larger than the
geometric effect due to the change of bandgap and inter-atomic spa-
cings. Bulk semiconductor strain sensor can have a very high sensi-
tivity, but they are not suitable for wearable applications due to limited
stretchability and flexibility. Stretchable polymer nanocomposite based
strain sensors combine the merits of elastomeric materials and con- Fig. 2. Current pathway within fractured GWF under stretched state.
ductive nanomaterials. The piezoresistive effect is low for composite Reproduced with permission (Li et al., 2012), Springer Nature.
strain sensors as the large mismatch of elasticity between conductive
network and elastomeric polymer leading to a relatively low adhesion. formulated an equation (Eq. (4)) to calculate the electric tunneling
resistance:
2.3. Disconnection mechanism
V h2d 4πd
Rtunnel = = exp ⎜⎛ 2mλ ⎞⎟
AJ 2
Conductive nanomaterials form a conductive network inside elas- Ae 2mλ ⎝ h ⎠ (4)
tomer matrix which produces signal relating to the strain. Electrons can
where J is tunneling current density, V is electrical potential, e is the
pass through the connection of overlapped nanomaterials within the
quantum of electricity, m the mass of electron, h Plank' constant, d the
percolation network. When the strain sensor is stretched, especially at a
distance between conductor and elastomer, λ the height of energy
large strain, the overlapped nanomaterials tend to disconnect as they
barrier of elastomer, and A for cross-section area of the conductor. Hu
have a much smaller elongation at break and a higher Young's modulus
et al. has conducted a comprehensive study on the tunneling effect on a
compared with elastomeric matrix. The disconnection of conductive
carbon nanotubes (CNTs)/polymer nanocomposite strain sensor (Hu
nanomaterials blocks the pathway of electrical connection, conse-
et al., 2008). For a small CNT volume fraction, the piezoresistivity is
quently decreases the conductivity of the strain sensor. As the strain
weak while tunneling effect is considered to be the principal me-
increases, the effect of disconnection mechanism increases as more
chanism of the sensor under small strain observed both from experi-
overlapped nanomaterials slip until a critical strain is reached where
ments and numerical simulation.
resistance goes infinity. The performance of strain sensor greatly relies
on disconnection and reconnection process. Permanent disconnection
3. Performance and features of strain sensors
of overlapped nanomaterials causes the irreversible degradation of
strain sensing accuracy.
To design a high-performance strain sensor, performance metrics
include but not limited in sensitivity (i.e. Gauge Factor, GF), linearity,
2.4. Crack propagation stretchability, response speed, durability, hysteresis, fabrication cost,
simplicity, safety, ease of packaging and some preferable features such
Fatigue crack propagation is the most common type of structural as self-healing, self-cleaning, self-powering, transparency, printability,
failure caused by static or cyclic loadings, especially for polymers etc.
(Ramsteiner and Armbrust, 2001). Cracks are initiated at points of high
stress and defects. During the subsequent stretching, the initiated cracks 3.1. Gauge factor (Sensitivity)
will grow and propagate till at a point the material suffers fracture.
Within the critical strain and attributed to viscoelastic polymer matrix, The simplest performance metric is the gauge factor (GF) which
the electrical conductivity is limited by crack propagation in nanoma- describes the slope of the relative change of electrical signal (resistance
terials and strain sensor is able to resume its initial conductivity by or capacitance) vs. applied strain, seen below in Eq. (5):
closing the cracks when applied strain is removed. This crack propa-
gation mechanism is more dominant for 2D nanomaterials such as ∆R ∆C
GF = , GF =
graphene or polymer thin films than 1D nanowires. Kang et al. reported R0 ε C0 ε (5)
an ultrasensitive graphene-on-polymer strain sensors with a gauge Where ΔR or ΔC is change of resistance or capacitance, R0 or C0 is the
factor of 6 × 106 at 8% strain (Li et al., 2012). A graphene woven initial resistance or capacitance at strain ε = 0%, and ε is the applied
fabrics (GWFs) prepared from chemical vapor deposition (CVD) was strain. GF represents the sensitivity of a strain sensor. Conventional
placed on top of elastomeric poly(dimethylsiloxane) (PDMS). By ap- metallic foil and semiconductor based strain gauge possess a relatively
plying strain around 1–8%, a significant amount of cracks in GWFs were high GF (2–5 for metal foil and 100–1000 for semiconductors) while the
initiated, propagated, and broke causing a significant resistance limitation in stretchability make them impractical for wearable devices.
change. The current pathway through a fractured GWF is shown in With the recent developments of nanotechnology and microelectronics,
Fig. 2. highly stretchable strain sensors with superior GF values have been
continuously reported (Frutiger et al., 2015; Larimi et al., 2018;
2.5. Tunneling effect Slobodian et al., 2018; Yan et al., 2014). For capacitive-type based
strain sensors, the main sensing mechanism is geometric effect. The
For resistive-type polymer nanocomposite strain sensors, dis- limitation of geometric change have limit the GF value of capacitive-
connection mechanism typically has a dominant effect. However, when type strain sensor within 1. For resistive-type based strain sensors, the
the separation distance between conductive nanomaterials and polymer main mechanisms affect GF include disconnections between conductive
matrix is sufficiently small, electrons can pass through forming a blocks, crack propagation in the thin films, and tunneling effect. Con-
complete pathway through tunneling effect. John Simmons had siderable structure change leads to a significant change of resistance

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Table 2
Summary of some recent reported polymer nanocomposite based strain sensors.
Material Sensing Mechanisms Stretchability Gauge Factor

Ag NP-SBS (Park et al., 2012) Resistive 200% 25

Ag NW-PDMS (Kim et al., 2015) Resistive 35% 20
Ag-PU fiber (Ma et al., 2015) Resistive 150% 211
Crumpled graphene-PDMS (Yan et al., 2014) Resistive 100% 7.1
PEDOT:PSS-PU (Seyedin et al., 2014) Resistive 350% 6
Ag NP/CNT-PDMS (Takei et al., 2014) Resistive 2.4% 95
PEDOT: PSS-polyvinyl pyrrolidone (PVP) (Sun et al., 2013) Resistive 4% 360
Graphene-Plastic (Hempel et al., 2012) Resistive 2% 150
Ag NW-Hydrogel (Lee et al., 2012) Resistive 460% 1.52
Pt-PUA (Kang et al., 2014) Resistive 2% 2000
Graphene Mesh-PDMS (Li et al., 2012) Resistive 8% 6 × 106
AuNWs-Latex Rubber (Gong et al., 2015) Resistive 350% 9.9
Ag NW-Ecoflex (Yao and Zhu, 2014) Capacitive 50% 0.7
CNT-silicone (Cohen et al., 2012) Capacitive 100% 0.99
Ionic fluid-silicone (Frutiger et al., 2015) Capacitive 700% 0.35

which in turn results in a high GF value. Amjadi et al. designed a strain poor adhesion between conductive layer and polymer layer. Seyedin
sensor with a sandwiched structure of PDMS/Silver Nanowires et al. successfully fabricated a strain responsive polyurethane (PU)/poly
(AgNWs)/PDMS (Amjadi et al., 2014). The elastomer nanocomposite (3,4-ethylenedioxythiophene): polystyrene sulfonate (PEDOT: PSS)
based strain sensor showed a tunable GF within the range of 2–14 and a elastomeric composite fibers by wet-spinning techniques (Seyedin et al.,
maximum strain of 70%. The AgNWs layer endorsed the electrical 2014). The conductive PEDOT: PSS was homogenously dispersed in PU
conductivity to the sensor and the GF was controlled by the number matrix. The composite fiber shows an increased Young's modulus and
density of AgNW percolation network. Lower number density gives a yield stress but a decreased elongation at break due to the presence of
rising amount of disconnections between AgNWs which considerably conductive polymer. The electrical conductivity of ~ 25 S cm-1 can be
increases the resistance of the device giving a high GF value. Cai et al. achived at 25% loading. A model simulates the reversible and irrever-
designed a capacitive-type strain sensor based on CNT film on PDMS sible deformations of PEDOT: PSS conductive network within PU was
film. The sensor is found to detect strains up to 300% with excellent proposed. Lipomi et al. (2011) designed a strain sensor composed of
durability (Cai et al., 2013). The gauge factor is very close to 1 which is CNTs/PDMS. CNTs were spray-coated onto the pre-stretched substrate
the theoretical limitation value for capacitive-type strain sensor. and forming a spring-like structure after releasing the strain. The na-
notube film can accommodate strains up to 150% with an excellent
conductivity of 2200 S cm-1.
3.2. Stretchability

3.3. Linearity
As mentioned in introduction section, the stretchability of polymer
nanocomposite based strain sensor derived from elastomeric matrix
Linearity is another performance parameter for strain sensor. A
made of polymeric materials and stretchable structure of conductive
linear fit of gauge factor or change of resistance over applied strain can
network. Table 2 shows a summary of the materials selection, gauge
provide the strain sensor with high accuracy and simple calibration.
factor and stretchability of some recent reported polymer nano-
Unfortunately, most reported resistive-type strain sensor exhibit a poor
composite based strain sensors. 1D nanomaterials such as CNTs and
linearity, especially at large strain. The nonhomogeneous morphology
AgNWs are considered preferable than other nanomaterials such as
upon stretching is believed to be the main reason of nonlinearity.
carbon blacks (CBs), graphene, and silver nanoparticles (AgNPs) be-
Calibration curve is required to correlate the signal to strain value and
cause of their high aspect ratios, and capability to sustain a percolation
periodic recalibration is recommended. Yu et al. (2017) developed a
network at large strain. The selections of elastomeric polymer matrix
wearable strain sensor composed of carbonized nano-sponge en-
and conductive nanomaterials will be discussed in detail in Section 4:
capsulated by silicone rubber. Their sensor showed three different
Materials Selection for Stretchable Strain Sensors.
gauge factors (GF of 4.3, 18.4 and 8.4) for strain ranges of 0–10%,
For conductive nanomaterials including carbon nanomaterials,
10–25%, 25–40%, respectively.
metallic nanomaterials or conductive polymers, none of them is in-
Capacitive-type stretchable strain sensor showed an excellent line-
trinsically elastic enough to bear a strain over 5%. So a designed con-
arity as discussed in Section 2.1: Geometric Effect. But the linearity is
ductive network which can retain mearsurable electrical conductivity at
limited due to the variation of Poisson's ratio at large strain. Yao and
a high strain while effectively transfer the tensile stress to elastomeric
Zhu (2014) fabricated a highly stretchable pressure and strain sensor
matrix is needed. There are mainly two effective approaches in fabri-
based on AgNW/PDMS/Ecoflex films. The AgNW was patterned on
cating a stretchable strain sensor: 1. Simultaneous blending of con-
PDMS by screen printing, and ecoflex film as dielectric material was
ductive materials and stretchable matrix. 2. Construct a stretchable
orthogonally placed between two AgNW/PDMS films. The sensor
conductive network (such as buckling, spring, coiled, and open mesh
showed a linear response to strains up to 50% with a GF of 0.7 (Fig. 3).
structures, etc.) embedded inside an elastic matrix. The first approach is
In addition, the sensor showed a fast response time of 40 ms and good
both simple and scalable while typically produces uniform nano-
pressure mapping function.
composites. However, there are issues need to be addressed including: a
homogeneous dispersion should be achieved for good linearity of
signal, an insulating polymeric matrix reduces the conductivity of the 3.4. Hysteresis
device, a high percolation threshold needs a relative high loading of
conductive fillers, etc. The second approach can provide high con- Hysteresis is an important metric for wearable strain sensors espe-
ductivity, especially at large strain compared with the first method. But cially when monitoring dynamic motions such as walking, running,
the fabrication procedure is generally more complex, the stretch di- speaking, heartbeat, breathing, etc. For capacitive-type strain sensors,
rection is often limited, and mechanical property can be low due to the the hysteresis is usually negligible while resistive-type strain sensors

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Fig. 3. Strain sensing performance: a) Linear fit of strain sensing capability of the capacitive sensor up to 50%. b) Relative capacitance change for 1st and 100th
stretching of the capacitive sensor. Reproduced with permission (Yao and Zhu, 2014), Royal Society of Chemistry.

Fig. 4. Hysteresis: a) AuNWs-latex

rubber sensor: Resistance change as a
function of strain at 3 mm S-1 ex-
hibiting hysteresis of resistance change.
Reproduced with permission (Gong
et al., 2015), John Wiley & Sons. b)
CNT-PDMS sensor: Relative capaci-
tance change as a function of strain
with negligible hysteresis. Reproduced
with permission (Cai et al., 2013),
Springer Nature.

typically suffer large hysteresis (Fig. 4) (Gong et al., 2015; Yao and Zhu, ionic bond (Xu et al., 2016), metal coordination (Li et al., 2016a), etc.
2014). Capacitive-type strain sensor relies on the geometry of over- On the contrary, extrinsic self-healing materials rely on external healing
lapped dielectric layer between two electrodes. Though polymeric agents to repair damages. Extrinsic self-healing can self-heal their da-
elastomer is known for elastic hysteresis caused by energy dissipation mage by taking advantage of healing agents encapsulated in vehicles
due to material internal friction. However, because capacitance is di- such as microcapsules/microvascular (Patrick et al., 2014; Zhu et al.,
rectly related to the strain, not stress, based on Eq. (2), the effect of 2015), and guest/host structures (Highley et al., 2015). When there is a
stress-strain loop caused hysteresis is negligible. For resistive-type crack or damage, incorporated healing agents are released and diffused
strain sensor, because of their unique conductive mechanisms, the to the damaged areas to repair defects.
stretchable conductive network needs time to slide back to its original To create self-healable strain sensors, self-healing properties and
position. Higher frequency is likely to cause incomplete deformation sensing properties should be incorporated into one device. Based on the
leading to an amplitude decay. The stronger binding with the matrix intrinsic self-healing concept, Kuang et al. utilized a shape memory
can help reduce the effect of hysteresis (Gong et al., 2015). polymer, and developed a novel 3D printable semi-interpenetrating
polymer network (semi-IPN) elastomer ink using photocurable resin
(aliphatic urethane diacrylate) and thermoplastic polymer (poly-
3.5. Self-healing caprolactam, PCL) (Kuang et al., 2018). After 3D printing and UV ir-
radiation, semi-IPN polymeric structure showed excellent flexibility
Self-healing materials have attracted tremendous attention in var- and strechability up to 600% (Kuang et al., 2018). When the film was
ious fields due to their great potential for structural restoration and scratched by a sharp blade, scratch could be healed by heating the film
function recovery after mechanical damage (Kuang et al., 2018; Liu at 80 °C for 20 min in an oven. This self-healing behavior originated
et al., 2018; Wang et al., 2018a; Yang et al., 2018b). When materials are from entanglement of polymer chains and hydrogen bonding between
used for a long time, they are often damaged caused by mechanical PCL and urethane (Kuang et al., 2018).
stress and/or harsh environment (e.g. temperature, pH, light, etc.) The application of external temperature to initiate the healing
which are responsible for the loss of stability and shortening cycle life. process may restrict the wide application of the film, which motivate
Self-healing materials can prevent or reduce damage and thereby ex- researchers to develop room temperature self-healable composites.
tend the durability and stability. Self-healing materials are usually ca- Wang et al. developed a highly stretchable and self-healable ternary
tegorized into two distinct systems: intrinsic and extrinsic self-healing polymer (polyaniline/polyacrylic acid/phytic acid, PANI/PAA/PA)
materials (Liu et al., 2017). Intrinsic self-healing materials can heal the hybrid via a facile in-situ polymerization process, which can heal the
damage through inherent reversible bond without additional self- cracks at ambient temperature (Wang et al., 2018a). The fabricated
healing agents. Intrinsic self-healing processes can be accomplished ternary system exhibits high stretchability (500%) and electrical con-
through dynamic physical or chemical interactions including dynamic ductivity (0.12 S cm-1). The polymer composites showed excellent self-
covalent bond (Lai et al., 2016), polymer chains entanglement, hy- healing properties at ambient temperature (60% Relative Humidity &
drogen bond (Tee et al., 2012) and non-covalent interactions such as

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25 °C) with mild pressure to come in contact and 99% healing efficiency slip out and keep device surface clean and dry. However, combining
of mechanical and electrical properties through hydrogen bonding and high stretchability and superhydrophobicity is challenging. Cost is al-
electrostatic interactions after 24 h healing period (Wang et al., 2018a). ways a major consideration to commercialize wearable devices and
Similarly, Liu et al. (2018) also synthesized an ionic cross-linked make them available for most consumers. To achieve scalable produc-
double network (DN) hydrogel using polyethylene glycol (PEG)/poly tion, the design of fully printed electronics is desirable which help
(acrylamide-co-acrylic acid) (PAMAA) with Fe3+ infusion into the automate the fabrication process thus decreasing the cost and manu-
network with self-healing ability at room temperature. The resulting facturing the standardized products.
DN hydrogel can self-heal the impair because of reversible hydrogen
bonds and coordination bond, exhibiting impressive self-healing cap-
4. Materials selection for stretchable strain sensors
ability and high mechanical strength. The self-healing properties of the
DN hydrogel monitored using two pieces, one piece dyed with rhoda-
The recent advancement of materials science and nanotechnology
mine B, kept in contact for 12 h at room temperature. The healed hy-
have greatly contributed to develop next-generation high performance
drogel showed high stretchability (15 times higher) compared to pris-
wearable sensors that possess high flexibility, stretchability, and sen-
tine hydrogel indicates excellent healing efficiency. The incorporation
sitivity with wide detecting range. To obtain these desired properties, it
of Fe3+ ions also contributed increasing healing efficiency with the
is important to select suitable functional materials and rationally design
increase of the ions content (Liu et al., 2018).
their architectures. So far, various conductive nanomaterials have been
utilized for polymer nanocomposite based strain sensors, including
3.6. Transparency carbon blacks (CB) (Ke et al., 2017; Shintake et al., 2018; Wang et al.,
2018b; Wu et al., 2016; Zheng et al., 2015; Zhu et al., 2018), CNTs
Aesthetics also play a key role in the acceptance of wearable de- (Akhmadishina et al., 2013; Christ et al., 2017; Lin et al., 2017; Wang
vices. For most applicable scenarios of strain sensor, they can be seen by et al., 2014a; Zaporotskova et al., 2016; Zhang and Zhang, 2009),
others which means transparency is an attractive feature. Transparent graphene (Li et al., 2015; Liu et al., 2015; Wang et al., 2015; Yang et al.,
thin film wearables can be accepted by more consumers for catching 2017; Zhao et al., 2017b), AgNWs (Hu et al., 2010; Sinha et al., 2016;
less attention. There are many transparent polymeric elastomers but Wei et al., 2016; Zou et al., 2018), Cu nanowires (Cu NWs) (Hu et al.,
most conductive fillers are opaque especially carbon nanomaterials. 2014; Jason et al., 2016; Jung et al., 2016), Au nanowires (Au NWs)
Design an ultrathin film with low loading of transparent nanomaterials, (Wu et al., 2017), and conductive polymers such as polypyrrole (PPy)
such as doped graphene, AgNWs and conductive polymers, can help (Li et al., 2014; Yang et al., 2016), polyaniline (PANI) (Lin et al., 2017;
increase the transparency of stretchable conductive film (Zhao et al., Wujcik et al., 2014), and PEDOT:PSS (Choong et al., 2014; Lee et al.,
2017a). Lee et al. (2014) fabricated a CNTs/AgNWs/Ecoflex hybrid 2016; Zhan et al., 2017). These conductive materials provide electrical
nanocomposite with high flexibility, stretchability and transparency. conductivity that is the basis of sensing mechanism, but often show
The nanocomposites combine the enhanced mechanical compliance, unsatisfactory mechanical properties such as poor flexibility and
conductivity and optical transparency of small CNTs (d ~ 1.2 nm), and stretchability (Bae et al., 2013; Park et al., 2015a; Wang et al., 2014b).
the highly conductive AgNWs backbone to provide an efficient multi- For example, graphene can endure strain only up to about 7% that is far
scale electron transport path. The hybrid nanocomposite possesses a below the criteria for stretchable strain sensors. Therefore, it is desir-
transmittance over 90% and stretchability over 460% (Fig. 5). able to create hybrid composite materials having both high sensitivity
and good stretchability/flexibility (Amjadi et al., 2016). These two
properties can be attained by fabricating composites that consists of
3.7. Other features
electrically conductive fillers and elastomeric matrix, in which con-
ductive fillers provide sensing mechanism and elastomeric matrix en-
Some other favorable features include but not limited to powering,
dows desired mechanical properties. This part will introduce a couple of
self-cleaning, printability, etc. There have been very limited literatures
key stretchable/flexible matrix materials and electrically conductive
reporting stretchable strain sensors possessing these features. Wearable
materials considering their sensitivity, flexibility and stretchability.
devices require long power life with limited power supply while not
sacrificing performance. Most current wearable strain sensor uses data
acquisition devices connected by wires. Integration with power system 4.1. Stretchable/flexible elastomeric matrix
can free up wires making devices truly wearable. Self-cleaning surface
can keep wearable device clean despite its surroundings. It is especially Flexible matrices are supporting materials of strain sensors to pro-
important when used in sports or gaming situations where significant vide desirable mechanical flexibility and versatility. Ideally, flexible
amount of sweat is produced and could affect the accuracy of strain matrix materials should have good mechanical and thermal properties,
sensor. Self-cleaning surface with superhydrophobicity can help sweat chemical inertness, low cost, ease processability and good adhesion

Fig. 5. Surface plot of sheet resistance (a) and transparency (b) for different concentration of CNT/AgNWs concentration. c) High transparency of electrical con-
ductive CNT/AgNWs nanocomposite film. Reproduced with permission (Lee et al., 2014), John Wiley & Sons.

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Fig. 6. Illustration of highly stretchable carbon black

composite electrodes. a) Fabricated strain sensor. b)
Stretchability up to 500%. c) Structure of strain sensors
including electrode layers and dielectric layers. d) A smart
glove integrated with five strain sensors. Reproduced with
permission (Shintake et al., 2018), John Wiley & Sons.

with other functional materials. Most commonly used supporting ma- structure, PDMS/CNT/PDMS. The fabricated sensors showed relatively
terials include silicon based elastomers (such as PDMS) and rubbers, PU high stretchability (45% strain) and good sensitivity (GF of 35) with
foam (Chen et al., 2017; Hsu et al., 2017; Park et al., 2016), poly- excellent durability under cyclic loading-unloading. This sensor also
ethylene terephthalate (PET) (Hsu et al., 2017), polyimide (PI) showed a reliable sensing performance having less than 20% deviation,
(Kaltenbrunner et al., 2013), polyvinylidene fluoride (PVdF) (Zhou which indicates high accuracy of CNT/PDMS strain sensors to quantify
et al., 2017b), cotton (Li et al., 2017; Wu et al., 2016), paper (Li et al., strain-induced motions. Zhang et al. (2018b) demonstrated electroless
2016b), Ecoflex (Cheng et al., 2017; Lim et al., 2016; Ryu et al., 2015; deposition (ELD) of metals (Cu, Ni, and Ag) on functionalized PDMS
Zhang et al., 2017), Dragon skin (Cai et al., 2013; Cheng et al., 2017; substrates the with the aid of polydopamine to increase adhesion and
Frutiger et al., 2015), and Kevlar fiber (Lee et al., 2015a) for flexible stability for flexible and stretchable sensors. The polydopamine not
strain sensors. Among them, PDMS has been most widely used due to its only serve as the host material for metal ions to enhance the ELD
tunable mechanical properties, facile processability, chemical inertness, process but also play a vital role in bridging the meal film and the
low cost, and high tendency to adhere with other functional materials substrate. The fabricated conductive metal-polymer hybrid such as Ag-
(Larmagnac et al., 2014). The Young's modulus of PDMS matrix is much PDMS, Cu-PDMS and Ni-PDMS showed high electrical conductivity of
lower (around 0.4–3.5 MPa) (Amjadi et al., 2014; Fuard et al., 2008) 1.8 × 107, 1.2 × 107 and 0.7 × 107 S m-1, respectively. The as-pre-
compared with that of other matrices such as PU (15.1–151.4 MPa for pared Cu-PDMS showed stable metallic conductivity even after 5000
0.16 and 0.32 g cm-3 foam, respectively) (Patel et al., 2008), PI cycles at highest stretch strain (700%).
(84.1 GPa with 3.25% elongation at break) (Yang et al., 2018a), PVdF Besides PDMS, other silicone-based materials such as Ecoflex and
(0.84 GPa with 0.86% elongation at break) (Zhang et al., 2018a). This Dragon skin have been employed as elastomeric matrices because of
low Young's modulus indicates that PDMS can provide greater flex- their attractive mechanical properties; Young's moduli of Ecoflex and
ibility and versatility than other polymers. The Young's modulus of Dragon skin were 69 kPA and 152 kPA, respectively, which are even
PDMS matrix varies with the thickness of the membrane reported in the lower than PDMS (Amjadi et al., 2015; Cheng et al., 2017). Yu et al.
literature (Liu et al., 2009). Liu et al. found that the Young's modulus (2017) fabricated highly sensitive strain sensor using Ecoflex as a ma-
increases with the decrease of membrane thickness. The thinnest trix encapsulating carbon nanosponge. The fabricated composite
membrane (50 µm) showed 1400 KPa Young's modulus with the elon- showed excellent stretchability possessing high fracture strain up to
gation at break about 125% whereas the thicker membrane (1.8 mm) 600% with a reasonable GF ranging from 4 to 19. These sensors also
showed about 600 kPa. Owing to its low Young's modulus and high exhibited prompt response (< 100 ms) and excellent stability (> 1000
stretchability, PDMS is a great candidate as matrix in flexible strain cycles) with a wide frequency ranges from 0.01 to 1 Hz, indicating its
sensor fabrication (Liu et al., 2009). Wang et al. incorporated CNT into great potential as a skin wearable sensor.
PDMS substrate using digitally operated printer to fabricate multi-
directional CNT/PDMS strain sensors with high stretchability and sen- 4.2. Electrically conductive materials
sitivity. CNT ink dispersed with a surfactant, Triton X, were deposited
on the surface modified PDMS substrates through spray deposition, Carbon-based nanomaterials such CBs (Ke et al., 2017; Shintake
followed by additional PDMS coating, which gives a sandwich et al., 2017; Wu et al., 2016; Zheng et al., 2015; Zhu et al., 2018), CNTs

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(Akhmadishina et al., 2013; Christ et al., 2017; Lin et al., 2017; Wang electrical, optical and mechanical properties. Chun et al. (2017) pro-
et al., 2014a; Zaporotskova et al., 2016; Zhang and Zhang, 2009) and posed graphene (SLG & graphene flake) based sensors on stretchable
graphene (Li et al., 2015; Liu et al., 2015; Wang et al., 2015; Yang et al., PDMS substrate which can detect very low strains (around 0.1%) with
2017) possess high electrical, thermal conductivity, and excellent me- minimum resistance change. Various human body motions such as
chanical strength. When used as conductive fillers, the dimensionality stretching, bending and torsion were successfully monitored. The
of carbonaceous materials affects electrical and mechanical properties twisted shaped SLG patterned strain sensor exhibited stretchability up
of the composites. The polycrystalline and layered structure of CB to 20% with a gauge factor of 42.2 and bi-directional sensing ability. To
empower it as a prominent candidate for conductive network of the further improve sensitivity, Lee et al. (2017) fabricated graphene-based
composites with high electrical and thermal conductivity. Additionally, grid patterned sensors on stretchable PDMS polymer substrates via
CB possesses low density, chemical inertness and low cost, which are solution dipping layer-by-layer assembly. The layer-by-layer assembly
also advantageous characteristics as a filler material in elastomeric allowed precise thickness control of the film at molecular level to tailor
matrix to fabricate stretchable strain sensors (Ke et al., 2017; Shintake the electrical conductivity and sensitivity of the sensors. They con-
et al., 2017; Wang et al., 2018b; Wu et al., 2016; Zheng et al., 2015; Zhu cluded that the mechanical tolerance of the sensors increases with the
et al., 2018). With the addition of appropriate amount of CB particles, it increase of graphene layer thickness. The 7 bilayer of layer-by-layer
is possible to fabricate piezoresistive polymer (silicone, epoxy, PDMS) coating exhibited electrical failure at 45% strain with a compromised
composites for strain sensing applications (Shang et al., 2016). Shintake sensitivity, which indicates sensitivity is a function of the graphene
et al. fabricated CB-Ecoflex elastomeric composites that have high layer thickness (Lee et al., 2017). To investigate the subtle and large
stretchability up to 500% via film casting and CO2 laser ablation pro- human body motions, it is necessary to widen the strain range and in-
cess (Fig. 6) (Shintake et al., 2018). The fabricated composite allowed crease sensitivity limit of the strain sensors. Tao et al. (2017) applied a
the sensors to monitor the strain through either capacitance or re- one-step direct laser patterning method to fabricate Graphene/Ecoflex
sistance. The authors found that the capacitive-type sensor exhibited based strain sensor with high GF at high strain range. They found that
better performance compared with resistive-type sensor in terms of the fabricated graphene encapsulated Ecoflex sensor showed an ultra-
physical and mechanical compliances except Gauge Factor. The capa- high GF of 457 at 35% strain and GF of 268 at 100% strain with ex-
citive sensor showed high linearity (R2 = 0.9995), low hysteresis and cellent repeatability which significantly exceeds some reported value
high repeatability with consistent strain rates as high as 50% s-1. When (Zhao et al., 2012).
the addition of porous CB nanoparticle exceeds the percolation limit, Yan et al. (2018) fabricated flexible strain sensor using carbon/
can decrease the resistance performance by 7 orders of magnitude for graphene composites nanofiber yarns (CNY) and thermoplastic poly-
strain sensors. These sensors can repeatedly be used over 10,000 cycles urethane (TPU) via electrospinning method. They found that the per-
without mechanical and electrical failures. formance of the sensor depends on the structural parameters such as
CNTs is a one-dimensional sp2 carbon materials that possess high yarn quantity and thickness of substrate. The tradeoff between the TPU
aspect (length/diameter) ratio, low density. High tensile strength and film thickness and the sensitivity and stability of the sensors incited the
superior electrical conductivity proved them excellent candidate for author to find out the optimum structural conditions. The sensor ex-
sensors as prominent functional materials. CNTs-based polymer hybrids hibits an average gauge factor above 1700 under 2% strain at an op-
also showed superior sensing performance than the single component- timum yarn number and substrate thickness are 4 and 129 µm, re-
based strain sensors due to their improved mechanical and electrical spectively (Yan et al., 2018).
properties (Wujcik and Monty, 2013). Additionally, these properties of Besides carbon-based nanomaterials, metal nanostructures such as
conductive polymer nanocomposites can be tailored depending on as- metal nanoparticles, nanowires can also be utilized as a conductive
pect ratio and wall thickness of CNT as well as composition of com- material for strain sensors. As it is challenging to maintain both high
posites. electrical conductivity and flexibility of the device simultaneously,
Recently, CNT-based polymeric strain sensors with high sensitivity composites approach is similarly preferable. Wei et al. (2017) reported
and stretchability have been reported. Zheng et al. (2018) fabricated piezoresistive-type hybrid sensors based on biodegradable cotton fiber,
PDMS based CNTs-CB/PDMS elastomeric composites via solution AgNWs and rGO. The inherently rough surface of cotton fiber act as the
mixing casting method which exhibited excellent stretchability (300%), backbone and flexible substrate whereas implanted AgNWs act as
sensitivity, repeatability and reproducibility in a wide range of strain conductive bridge toward damaged rGO under tensile loading. Due to
(up to 200%). The hybrid sensors also exhibited outstanding stability the dynamic bridging nature of AgNWs, the fabricated sensor exhibited
even after 2500 cycles which allows reliable detection of human joint very low detection limit (0.125 Pa) and high stability (> 10,000 fatigue
motion such as the motion of finger, wrist, elbow and knee (Zheng cycles) (Wei et al., 2017). Lee et al. (2015b) fabricated AgNWs and
et al., 2018). AgNPs based highly stretchable strain sensor incorporated in a styr-
Christ et al. (2017) successfully 3D printed an elastic strain sensor ene–butadiene–styrene (SBS) elastomeric substrate via spinning
using thermoplastic polyurethane and multiwalled carbon nanotube method. The fabricated sensor showed high elongation at break (~
(MWCNT). They utilized the 3D printing process using extruded fila- 900% strain) and excellent electrical conductivity (2450 S/cm) because
ment of TPU/MWCNT to achieve sensing capability with high me- of high conductivity of AgNWs and high stretchability of SBS matrix.
chanical properties. The printed materials loaded with 2% MWCNT During tensile stress, the embedded AgNWs come across and bridge the
showed a highest gauge factor of 176 at 25% applied strain, but the 3% high resistive gap between AgNPs, maintaining the conductivity of the
MWCNT loaded sample offered the optimum mechanical and electrical device and stretchability at a high strain. They also found that the
properties up to 100% strain. conductivity of the device increased with the fiber length at a perco-
Zhou et al. (2017a) developed ultrasensitive strain sensors using lation threshold limit of 20 µm (Lee et al., 2015b).
single walled carbon nanotube (SWCNT) embedded in PDMS film. The Conductive polymers such as polypyrrole (PPy) (Li et al., 2014;
fabricated sensor shows high strain levels with a gauge factor of over Yang et al., 2016), polyaniline (PANI) (Lin et al., 2017; Wujcik et al.,
107 at 50% strain. This extremely high sensitivity might be ascribed to 2014), and PEDOT:PSS (Choong et al., 2014; Lee et al., 2016; Liu et al.,
the low electrical resistance of SWCNT, which maximize a change of 2011; Zhan et al., 2017) have also attract extensive attention in wear-
resistance in cracked region of the composites. PDMS film plays the key able strain sensor research due to their ease of preparation, inherent
role in providing flexibility and stretchability of the film as CNTs alone flexibility, low Young's modulus, and good adhesion with elastomeric
do not have satisfied stretchability. matrix. However, conductive polymer based composites tend to have an
Graphene is an emerging two-dimensional carbon material that can inferior conductivity compared with carbon and metal nanofiller based
be a prominent candidate for strain sensors because of its attractive composites. Some researchers have reported strain sensors with

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conductive nanofiberous network based on electrospun conductive wearable strain sensor with power, signal conditioning, communica-
polymers. Liu et al. fabricated a novel strain sensor based on PEDOT: tion, and data management units into a complete system. The integra-
PSS/Polyvinyl Alcohol (PVA) nanofibers on Kapton substrate (Liu et al., tion of the whole system with high reliability, robustness, long power
2011). The conductivity can be tuned by controlling the concentration life has not been reported yet and needs multidisciplinary teams to
of the additive dimethylsulfoxide from 4.8 × 10-8 to 1.7 × 10-5 S cm-1. address this issue. Finally, some features are attractive and technical
Though the sensor shows excellent stability and high GF of 396, the issues needs to be tackled when adding into strain sensors. Examples
stretchability is limited at 1.2% due to the nature of nonwoven nano- are self-healing, self-powering, self-cleaning, transparency, biodegrad-
fiberous network. Bin et al. adopted a novel reciprocating-type elec- ability, etc., some have been discussed in Section 3. Further investiga-
trospinning setup to produce PEDOT:PSS/PVP nanofibers with curled tion and cooperation of researchers in material science, nano-
architectures (Sun et al., 2013). The GF (which is 360) is close to Liu's technology, microelectronics along with industrial companies are
report but the stretchability was enhanced to 4%. Seyedin et al. (2014) needed to overcome these challenges.
successfully dispersed PEDOT:PSS homogenously in PU elastomer
which greatly enhance the sensor stretchability to over 300%. This Acknowledgements
study has been discussed in Section 3.2: Stretchability.
This research did not receive any specific grant from funding
5. Conclusions and outlook agencies in the public, commercial,or not-for-profit sectors.

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