Applied Nanoscience

https://doi.org/10.1007/s13204-019-01032-2

ORIGINAL ARTICLE

Functional nanocomposites for 3D printing of stretchable

and wearable sensors
Mohammad Abshirini1 · Mohammad Charara1 · Parisa Marashizadeh1 · Mrinal C. Saha2 · M. Cengiz Altan3 ·
Yingtao Liu4 

Received: 12 February 2019 / Accepted: 9 April 2019

© King Abdulaziz City for Science and Technology 2019

Abstract
This paper presents highly flexible strain sensors fabricated by extrusion-based 3D printing of electrically conductive nano-
composites consisting of multi-walled carbon nanotube (MWNT)/polydimethylsiloxane (PDMS). The effects of printing
parameters and nanocomposite formulation on the piezoresistive behavior of the 3D-printed sensors are investigated. Experi-
mental results demonstrate that the 3D printing-induced alignment of MWNTs results in the enhancement of piezoresistive
sensing function of the nanocomposites. Detailed analyses are performed using the optimized sensors to characterize their
sensing performance, including load rate dependency, repeatability under long-term cyclic loads, and relaxation behavior.
The 3D-printed strain sensors demonstrate high flexibility, stretching to 146% strain before fracture, and exhibit a linear
piezoresistive response up to 70% strain with a gauge factor of 12.15. The distribution of nanotubes in the polymer and
the piezoresistive mechanism of the material are explored by in situ micro-mechanical testing under a scanning electron
microscope (SEM). The developed sensors are attached on gloves to monitor the motion of a human hand, demonstrating
their application wearable electronics.

Keywords  Piezoresistivity · Stretchable sensors · 3D printing · Carbon nanotube · Conductive nanocomposites

Introduction
Recent scientific progress in the use of electronic devices
for strain sensing applications has attracted significant
attention in the fields of soft robotics (Fallahi et al. 2017;
Zheng et al. 2015), electronic skins (Ho et al. 2016; Hong
Electronic supplementary material  The online version of this
article (https​://doi.org/10.1007/s1320​4-019-01032​-2) contains
supplementary material, which is available to authorized users.
* Yingtao Liu
yingtao@ou.edu
1
School of Aerospace and Mechanical Engineering,
University of Oklahoma, 865 Asp Ave. #301C, Norman,
OK 73019, USA
2
School of Aerospace and Mechanical Engineering, University
of Oklahoma, 865 Asp Ave. #208, Norman, OK 73019, USA
3
School of Aerospace and Mechanical Engineering, University
of Oklahoma, 865 Asp Ave. #205, Norman, OK 73019, USA
4
School of Aerospace and Mechanical Engineering, University
of Oklahoma, 865 Asp Ave. #218A, Norman, OK 73019,
USA
et al. 2016; Martinez et al. 2013), and wearable devices for
human health monitoring (Amjadi et al. 2014; Choi et al.
2017; Trung et al. 2017). These applications require flexible
strain sensors with high sensitivity and durable performance.
In general, strain sensing range and sensitivity are two key
parameters used to evaluate the quality of these sensors. Par-
ticularly, the sensitivity is quantified in the form of gauge
factor (GF), and is defined as the ratio of relative electrical
resistance change to applied strain. Conventional metallic
strain gauges offer a low GF (around 2) and a limited sens-
ing range (< 5% strain), while semiconductor-based sensors
offer high GFs but a limited detection range, making neither
of them suitable for wearable sensing applications (Zhang
et al. 2017).
Elastomeric nanocomposites enhanced by conductive
nanofillers are one of the most popular advanced materials
for stretchable strain sensing applications. Polydimethylsi-
loxane (PDMS) (Chowdhury et al. 2018; Lu et al. 2012),
polyurethane (Zhang et al. 2013), and natural rubber (Selvan
et al. 2016) have been employed as elastomeric polymers
in these nanocomposites. The addition of conductive nano-
fillers to these flexible matrices endows the base material

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with electrical properties which can be exploited to meas-
ure its deformation. Both capacitance-based and resistance-
based strain sensing mechanisms have been reported in
literature, though the electrical resistance-based method
has been more commonly reported (Abshirini et al. 2018;
Cao et al. 2015; Luo et al. 2018). The change in electrical
resistance is believed to be induced by the reorganization of
the electrically conductive network formed by nanofillers
under mechanical stimulus (i.e., tension or compression).
Researchers have explored a variety of nanofillers, including
carbon black (Zheng et al. 2017), carbon nanofiber (Charara
et al. 2019b; Chowdhury et al. 2016), graphene (Park et al.
2015), and carbon nanotubes (CNTs) (Ryu et al. 2015; Liu
et al. 2012), to increase the conductivity of elastomers. Of
these, multi-walled carbon nanotubes (MWNT) have been
widely used to improve these polymers’ conductivity due
to their excellent electrical characteristics at low concentra-
tion (Hu et al. 2008; Kang et al. 2006; Lipomi et al. 2011).
Piezoresistive response in nanocomposite materials has been
previously observed (Obitayo and Liu 2012). By measuring
the electrical resistance change resulting from mechanical
deformation in these materials, the applied strains can be
calculated.
Numerous studies have been performed in recent years
to produce a sensor with the capability of detecting strains
up to 100%. However, in most of the cases, these sensors
exhibit a non-linear sensing response over a wide strain
range (Liu et al. 2015; Yamada et al. 2011) and a low GF at
large strains (Cai et al. 2013; Cohen et al. 2012; Liu et al.
2015; Yamada et al. 2011). Recently, several approaches
have been developed to fabricate sensors with high sensi-
tivity and stretchability, such as micro/nanocracking-assisted
conductive network resulting in sensors with high GFs but
very low sensing range (Chen et al. 2016; Hoang et al. 2016;
Kang et al. 2014) and the creation of porous nanocomposite
materials (Li et al. 2017; Liu et al. 2016; Wu et al. 2017).
However, the fabrication process to create such sensors is
often highly complex and time consuming. Therefore, it is
important to explore a novel strain sensor fabrication tech-
nique which allows for the facile manufacturing of highly
stretchable, durable sensors with a wide sensing range.
Most reported nanocomposite strain sensors were manufac-
tured by molding and casting (Amjadi et al. 2016; Obitayo and
Liu 2012). Recently, various additive manufacturing methods
have been used for fabricating conductive polymers. Fused
deposition modeling, based on the melting of thermoplastic
filaments to manufacture a desired 3D model, has been widely
used for the printing of conductive thermoplastic polymers
(Costa et al. 2014; Gnanasekaran et al. 2017; Kumar et al.
2018; Kwok et al. 2017; Leigh et al. 2012; Wei et al. 2015;
Yu et al. 2017). Other printing techniques have been used for
manufacturing conductive polymers, including inkjet printing-
based deposition of ink droplets (Michelis et al. 2015), aerosol
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Applied Nanoscience
jet printing (Agarwala et al. 2018; Goh et al. 2018a), and direct
writing (Kim et al. 2012; Vatani et al. 2013). Recently, extru-
sion-based 3D printing technology has been reported as a rap-
idly expanding approach to fabricate customizable structures
and prototyping of elastomers, such as PDMS, and related
elastomeric nanocomposites (Charara et al. 2019a; Guo et al.
2017; Hwang et al. 2018; Truby et al. 2018). Due to its thixo-
tropic flow properties, PDMS can be 3D printed under ambi-
ent conditions and used to create relatively thin multi-material
devices, such as a bionic ear (Mannoor et al. 2013). Although
the printed PDMS is able to maintain its geometric fidelity
after curing, the low elastic modulus of the pre- and post-cured
PDMS and its deformation under gravity prior to curing still
restricts the 3D geometries that can be fabricated due to its
inability to maintain shape fidelity directly post deposition.
Hinton et al. reported a 3D printing method for PDMS in a
hydrophilic support bath, aiming to enable true freeform fab-
rication of complex structures (Hinton et al. 2016). Dispersion
of nanoparticles in PDMS can significantly improve materi-
als’ elastic modulus and viscosity, leading to 3D printable and
highly elastic nanocomposites. Carbon-based nanoparticles,
including graphene and CNTs, have been dispersed in elasto-
mers and 3D printed for electronic and biomedical applications
(Jakus et al. 2015; Wang et al. 2017). Most previous work
has focused on nanocomposite characteristics, 3D printability,
and potential applications. However, there is a lack of studies
exploring the effects of 3D printing and curing parameters
on the nanocomposite’s properties and sensing response due
to the various nano- and micro-structures formed within the
material during the manufacturing process (Goh et al. 2018b).
In this study, an electrically conductive nanocomposite is
3D printed on a pristine elastomer substrate to fabricate highly
stretchable and wearable strain sensors. To obtain optimal
piezoresistive sensing function, nanocomposites are printed
varying processing parameters, including needle diameter,
curing temperature, and MWNT concentrations. All the
printed materials are tested under cyclic tensile load to iden-
tify their sensitivity and linear sensing response range. The
optimized sensors are further tested to validate their reliability
and repeatability under various cyclic loads and loading rates.
The piezoresistive sensing mechanism was demonstrated by
comparing the MWNT conductive network using in  situ
micro-mechanical testing in a scanning electron microscope
(SEM). Finally, the fabricated sensors are used as wearable
sensors to detect the motions on a human hand and fingers.
Experimental
Materials
Unless otherwise stated, all the materials in this study were
used as received. SYLGARD 184 PDMS base elastomer
Applied Nanoscience
(part A) and curing agent (part B) were purchased from Dow
Corning. MWNTs with an average aspect ratio of 100 and
diameter of 50–90 nm were purchased from Sigma-Aldrich.
Tetrahydrofuran (THF) purchased from Sigma-Aldrich was
used as the solvent.
Preparation and 3D printing of nanocomposites
Pristine PDMS sheets were first manufactured using an alu-
minum mold. The PDMS prepolymer was prepared by mix-
ing the base elastomer and curing agent at the 10:1 part A to
part B weight ratio, as recommended by the manufacturer.
The mixed prepolymer was degassed in a vacuum desicca-
tor at room temperature for 30 min and cured in an oven at
65 °C for 4 h. The manufactured pristine PDMS sheets were
used as substrates during the 3D printing process.
The electrically conductive nanocomposites were pre-
pared by dispersing MWNT in the PDMS base elastomer
using the solvent-assisted ultrasonication method. MWNT
and PDMS base elastomer were added into 30 ml THF and
mixed for 5 min using a magnetic stirrer at 350 RPM. After
mixing, a 750 watt probe sonicator was used to sonicate
the PDMS base elastomer/THF/MWNT solution for 30 min.
The mixture was kept on a hot plate at 65 °C and stirred
at 100 RPM overnight to evaporate all the THF solvent.
Finally, the PDMS curing agent was added to the prepared
nanocomposites and mixed for 3 min before loading into a 3
mL syringe and 3D printing on the pristine PDMS substrate.
The schematic of the material preparation process is shown
in Fig. 1a. Nanocomposites with various MWNT concentra-
tions were printed and characterized to identify the optimal
nanocomposite formulation with the highest piezoresistive
sensing function.
A Tronxy X5S system was modified to 3D print the con-
ductive nanocomposites by installing a geared syringe pump
(Abshirini et al. 2018). Plastic syringes capped with needles
Fig. 1  Schematics of the a nanocomposite material synthesis and b strain sensor fabrication processes
of various diameters were used to print the nanocomposites
on pristine PMDS substrates. The prepared MWNT/PDMS
nanocomposites were printed into an electrically conduc-
tive pattern of two connected 30 mm long parallel lines.
The designed 3D model was converted into G-code using
the Repetier and Slic3r open source software. The extru-
sion pressure is adjusted based on the volumetric flow rate
required depending on the filament diameter (in this case the
syringe diameter) and the nozzle diameter (in this case the
needle diameter). For this work, printhead speed of 1 mm/s
is used to deposit the nanocomposite. The printed conduc-
tive pattern was cured at various temperatures (25 °C, 65 °C,
and 130 °C) in an oven to explore the curing temperature
effects on the obtained piezoresistive sensing function. A
layer of pristine PDMS was coated on the printed nanocom-
posites and cured at 130 °C for 20 min before mechanical
testing. The schematic of the strain sensor fabrication pro-
cess is illustrated in Fig. 1b. The modified 3D printer, the
printing process, and the final shape of the fabricated strain
sensor are shown in Fig. 2c. The dimensions of the final sen-
sors are 50 × 30 × 1.8 mm. The PDMS substrate and sealing
layer are both 0.9 mm.
Piezoresistive characterization
of the nanocomposite
Three parameters, including MWNT concentration, needle
diameters, and curing temperature were optimized to obtain
the highest piezoresistive sensing function of the developed
strain sensors. Cyclic tensile tests were performed for each
set of the fabricated strain sensors using an Instron single
column uniaxial test machine at maximum strains of 10, 15,
20, 25, and 30%. The electrical resistance of the tested sam-
ples was continuously recorded using an Agilent 34401A
multimeter during the mechanical tests for all samples. The
experimental setup is shown in Fig. 3. The load/unload
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 Applied Nanoscience

Fig. 2  a Modified 3D printer,

b depositing nanocomposite
on the PDMS substrate, c final
shape of the printed strain sen-
sor on pristine PDMS substrate
(ruler for scale shown in mil-
limeter and centimeter)

concentrations: 1.5 wt%, 2 wt%, 2.5 wt%, and 3 wt%.

Fig. 3  Experimental setup of piezoresistive sensing tests under cyclic
tensile load
procedure was repeated for six cycles to ensure the repeat-
ability of the sensing response in each test. The normalized
electrical resistance change was calculated to quantify the
sensing behavior of the 3D-printed sensors using Eq. 1.
R − Ro
Normalized resistance change = 100 × (%) (1)
Ro
where Ro is the initial electrical resistance of the sensor and
R is the real-time measured electrical resistance. In addition,
GF was calculated to quantify the piezoresistive sensitivity
of the 3D-printed sensors using Eq. 2.
( )
R−R0
All nanocomposite sensors were printed using a needle
of 0.41 mm diameter and cured at 130 °C. The optimal
nanocomposite with the highest piezoresistive sensitivity
was identified using the cyclic mechanical tests discussed
above. The nanocomposite with the selected CNT content
was used to print sensors using four needle diameters of
0.26, 0.41, 0.71 and 1.19 mm, cured at 130 °C, and tested
under the same cyclic load conditions as discussed above
to explore the effect of needle diameter on the proper-
ties of the printed nanocomposite sensors. Finally, the
nanocomposites printed with the optimal formulation and
needle size were cured at three different temperatures of
25 °C, 65 °C, and 130 °C to investigate the effect of cur-
ing temperature on their piezoresistive sensing function.
Nanocomposite sensors printed using all the optimized
parameters and formulations were tested to evaluate their
sensing reliability and repeatability. Uniaxial tensile loads
at the rate of 1 mm/min were applied to identify the max-
imum strain that the sample carried before fracture. In
addition, cyclic tensile loads were applied to find the maxi-
mum strain range in which the sensor showed a linear pie-
zoresistive response. Moreover, the load rate dependency
of the printed sensors was investigated under cyclic tensile
load at loading rates varying from 5 to 200 mm/min, at a
constant 10% maximum strain. The piezoresistive sens-
ing response was recorded throughout all the experiments.
The long-term sensing and fatigue behavior of the printed
sensors was tested under tensile loads at a loading rate of
3 mm/min and 10% max strain for 400 cycles. Finally, the

GF =
R0 (2) stress and electrical resistance relaxation behaviors of the
𝜀 sensors were investigated by holding the sample at 10%
where ε (mm/mm) is the applied strain on the sample. strain load for 8000 s while recording electrical resistance
The effect of the MWNT concentration on the piezore- and stress data.
sistive behavior of the printed sensors was evaluated
by testing nanocomposites with four different MWNT

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Applied Nanoscience
In situ characterization of the piezoresistive sensing
mechanism
Understanding the piezoresistive sensing mechanism is
critical for the optimization of 3D printed sensor behav-
ior. In this paper, in situ micro-mechanical tensile tests
were conducted to investigate the reorganization of the
electrically conductive MWNT network in the nano-
composites under tensile load. A printed nanocomposite
sensor was manufactured without a pristine PDMS seal-
ing layer, clamped on a micro-mechanical testing stage
(Gatan Microtest 200), and tested in an SEM (TESCAN
VEGA II), while SEM images were captured at different
strain increments, as shown in Fig. 4. The reorganization
of the MWNT network in the nanocomposite was dem-
onstrated by comparing the SEM images at 0% and 20%
strain.
Fig. 4  In situ SEM analysis of the strain sensor using  a micro-
mechanical tensile stage
Fig. 5  SEM images of the nanocomposite: a printed conductive nanocomposite on pristine PDMS substrate, b distribution of MWNT in the
PDMS matrix
Human body motion recognition
The feasibility of using the developed strain sensors as wear-
able sensors was explored. Five strain sensors were printed
and mounted on a glove to detect finger motions, and the
sixth sensor was attached on the wrist area to detect wrist
bending. Electrical resistance data were recorded throughout
the test to validate the sensors’ performance as wearable
electronic devices.
Results and discussion
Distribution of the nanocomposite pattern
in the sensor
Figure 5a shows the SEM images of the cross-section of the
strain sensor, detailing the MWNT distribution within the
printed nanocomposite. The half oval shape with a width of
598 μm and a height of 228 μm was the conductive nano-
composite embedded between two layers of pristine PDMS.
Due to surface wetting, the cured cross-section of the 3D
printed nanocomposite sensor was in the shape of half oval
instead of half circle, as outlined in Fig. 5a. Good disper-
sion of the MWNT in the PDMS matrix can be observed in
the high-magnification SEM image in Fig. 5b. No MWNT
agglomerates or fractured nanotubes were observed during
SEM imaging. The width and thickness of the deposited pat-
tern using different needles were measured from the SEM
images captured from cross-sections and tabulated in Table 1.
Optimization of MWNT concentration
in nanocomposites
To study the effect of MWNT concentration on the piezore-
sistive sensing function of the conductive nanocomposite,
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 Applied Nanoscience

Table 1  Width and thickness of the deposited pattern after curing nanocomposites with 3 wt%, 2.5 wt%, and 2 wt% MWNT
Needle size (mm) Width (mm) Thickness (mm) were 1.15, 1.56, and 2.51, respectively. However, the average
GF of nanocomposite with 1.5 wt% increased up to 12.98.
0.26 0.394 0.135 Nanocomposites with 1 wt% MWNT were also printed
0.41 0.598 0.228 and tested following the same testing procedure. However,
0.71 1.122 0.452 their poor electrical conductivity did not offer a measur-
1.19 1.861 0.736 able piezoresistive sensing function. Since the piezoresis-
tive sensing mechanism is due to the reorganization of the
conductive network of MWNTs under external load, an
appropriate amount of MWNTs can form the most effec-
tive micro-scale connections among MWNTs, resulting in
the nanocomposites being most sensitive to external loads.
Therefore, nanocomposites with 1.5 wt% MWNT are con-
sidered the optimal material for sensor development in this
paper.

Optimization of nanocomposite printing

parameters

The effect of the printing needle diameter was investigated

Fig. 6  The effect of CNT concentration on the strain sensing response
sensors fabricated with four different MWNT formulations
were tested via cyclic loading at max strains between 10 and
30% at a loading rate of 2 mm/min. The electrical resist-
ance changes of nanocomposites with various MWNT con-
centrations are shown in Fig. 6. By reducing the MWNT
loading, the piezoresistive sensitivity of the printed nano-
composites improved, as indicated by the increased slopes
at lower MWNT contents in Fig. 6. The average GFs of
by printing nanocomposites with 1.5 wt% of MWNT using
four different needle diameters. As shown in Fig. 7a, the
increased needle diameters resulted in wider nanocomposite
patterns. The piezoresistive sensing function of these sen-
sors is expected to be different, since the MWNT distribu-
tions and alignment in the nanocomposites can be affected
by the shear flow generated during the printing process. The
measured piezoresistive sensing functions of the four types
of sensors tested under 10–30% strain are shown in Fig. 7b.
It should be noted that the piezoresistive sensitivity was
enhanced by reducing the needle diameter from 1.19 mm to
0.41 mm. The average GF is 13.01 for the sensors fabricated
with needles of 0.41 mm diameter compared to 1.92 for the
sensors printed using 1.19 mm diameter needles.

Fig. 7  a Printed sensors of various widths due to the effect of needle diameter, b piezoresistive sensing function of sensors printed by various
needle diameter

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Applied Nanoscience

The effect of needle diameter on the piezoresistive sens-

ing function can be due to the alignment of the MWNT
and formation of the conductive network within the printed
nanocomposites. During the printing process, the flow rate
of nanocomposites near the needle wall was lower than that
near the center of the needle, resulting in the shear stress
within the nanocomposite caused by the extrusion. The shear
stress at a surface element parallel to the needle wall can be
written as:
𝜕u
𝜏(y) = 𝜇
𝜕y (3)

where μ is the dynamic viscosity of the flow, u is the flow

velocity along the needle wall, and y is the distance away
from the needle wall. Shear stress caused by shear flow can
align MWNT nanoparticles along the printing direction, as
shown in Fig. 8. Since the same amount of MWNT nano-
composites was printed due to the constant extrusion motor
speed, the generated flow rate and shear stress using smaller
needles were higher than those using larger needles, result-
ing in better alignment of MWNT within nanocomposites.
Similar phenomena have been reported in literature when
micronozzles were used to deposit nanofillers in nanocom-
posites (Compton and Lewis 2014; Farkash and Brandon
1994; Shofner et al. 2003). However, if the needle diameter
is too small, the printed nanocomposite sensors may have
discontinuous MWNT alignment and MWNT breakage
during printing, resulting in reduced piezoresistive sensing
function. The poor sensing behavior can be more significant
under high tensile strains. This is evident by the non-linear
response of the 0.26 mm needle size after 20% strain, which
is likely due to poor and disrupted MWNT network in this
sensor under high extension condition.
The curing temperature effect on the piezoresistive sens-
ing function was characterized by printing sensors using the
1.5 wt% MWNT nanocomposite and a 0.41 mm needle, and
immediately curing the printed nanocomposites at three dif-
ferent temperatures of 25 °C, 65 °C, and 130 °C. Figure 9
shows the piezoresistive response of these samples tested
under 10–30% of tensile strain. The piezoresistive sensitivity
Fig. 9  Effect of curing temperature on the piezoresistive sensing
function
of the printed sensors was reduced when low curing temper-
ature was used. The average GFs of nanocomposites cured at
25 °C, 65 °C, and 130 °C were 1.8, 7.98, and 12.91, respec-
tively, when tested under 10–30% of tensile strain. It should
be noted that it only took 10 min to fully cure the printed
nanocomposite at 130 °C, compared to 96 h when cured at
25 °C. Hence, it can be estimated that the alignment of the
MWNTs was disrupted during the long curing process when
a low curing temperature was employed. To take advantage
of CNT alignment generated during the printing process, the
microstructure of the conductive MWNT network should be
“locked” quickly by curing the nanocomposites as quickly
as possible. The ideal curing process should be the in situ
curing of nanocomposites during the printing. Otherwise,
the initial orientation of the MWNTs in the nanocomposites
can change and reduce the piezoresistive sensing function of
the printed nanocomposites.
According to the obtained results, the best piezore-
sistive sensing function can be achieved using the 1.5
wt% MWNT printed on the pristine PDMS substrate
using 0.41 mm needle and cured at 130 °C. The optimal

Fig. 8  Schematic of nanotube
alignment during the printing
and realignment during the
loading

13

nanocomposite formulation and manufacturing param-
eters were used to fabricate all the stretchable strain sen-
sors that were characterized in the following sections.
Fig. 10  a Printed sensor under 0% and 146% tensile strains; b Pie-
zoresistive sensing response of the flexible strain sensor from 10 to
70% tensile strain; c effect of loading rate on piezoresistive sensing
behavior and details of the relative piezoresistive change under load-
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Characterization of piezoresistive sensing function
To evaluate the maximum strain that the sensors carried
prior to fracture, continuous uniaxial tensile load was
applied at the load rate of 0.2 mm/min. Figure 10a shows
the sensor mounted on the Instron uniaxial test machine
before applying the load and the sensor at the moment before
ing rate of 5  mm/min, 25  mm/min, 50  mm/min; d durability test of
printed sensor for 400 cycles; e relaxation test showing the resistance
and stress change under 10% strain for 8000 s; f FE results showing
the strain distribution in the layers of the sensor at 40% strain
Applied Nanoscience
failure. The maximum strain the sensors carried was 146%
tensile strain, which was close to the reported maximum
strain that PDMS can sustain (elongation, 160%) (Cai et al.
2013). This high fracture strain allows the potential applica-
tion of the developed sensor under high strain conditions.
The piezoresistive response of the printed sensors at dif-
ferent max strains was characterized to identify the linear
strain sensing range. Cyclic tensile load tests at various max
strains were conducted starting from 10% strain, increment-
ing by 5% up to 70% strain. The piezoresistive response
of the sensor was measured continuously and is shown in
Fig. 10b. The electrical resistance of the nanocomposites
above 70% strain was beyond the working range of the mul-
timeter used in this study, therefore, the sensing performance
above 70% tensile strain is not reported in this paper. The
sensing results in Fig. 10b shows that the sensor exhibits a
linear response throughout the tested 10–70% strain range,
with an average GF of 12.15, which is about six times higher
than that of conventional metallic strain gauges (Yamada
et al. 2011). The wide linear sensing range (at least up to
70% tensile strain) with a high GF demonstrated the poten-
tial strain sensing capability under large deformations.
To evaluate the load rate dependency of the printed sen-
sors, cyclic tensile tests at 10% max strain were conducted
under various loading rates. As shown in Fig. 10c, the pie-
zoresistive response initially improved with the increased
loading rate, indicating enhanced piezoresistive sensitivity at
a higher loading rate, but the sensing behavior stabilized after
the loading rate reached 50 mm/min. This demonstrated that
the viscoelastic behavior of the material was affected at load-
ing rates of 50 mm/min or lower, with the effect disappear-
ing at loading rates of 50–200 mm/min. The detailed cyclic
piezoresistive response of the sensor for the tests at loading
rates of 5, 25, and 50 mm/min is also shown in Fig. 10c.
An important parameter to verify the robustness of a
strain sensor is its long-term sensing response. The piezore-
sistive behavior of the sensor under a tensile fatigue test of
400 cycles loaded up to 10% strain is shown in Fig. 10d.
The cyclic resistance change degraded gradually in the first
100 cycles and then became relatively stable. The reduction
occurred in both the peaks and valleys in the initial cycles.
The peak to valley resistance response was illustrated sepa-
rately for three different points throughout the test: cycles
20–25 (start), 200–205 (middle), and 380–385 (end). The
relative resistance that changed in the cycles of 20–25 was
around 5.1% higher than that of cycles of 200–205 and
380–384. This result shows the acceptable long-term per-
formance of the printed sensors.
To understand the relaxation behavior of the strain sensor,
a 10% strain tensile load was applied and held for 8000 s. The
sensor’s stress and resistance were recorded continuously by
the Instron test machine load cell and multimeter, respec-
tively. The normalized stress and resistance change (defined
as the change in the real-time value from the initial values,
divided by the initial value) throughout the experiment are
depicted in Fig. 10e. Both stress and resistance degraded due
to the viscoelastic behavior of the elastomer polymer in con-
stant extension. However, the stress reduction was around 8%
compared to 3.4% for the resistance, which revealed that the
relaxation behavior of the stress was higher than that of the
piezoresistance response, likely due to additional relaxation
in the pristine PDMS layers, and not the conductive pattern.
Finite element analysis (FEA) simulations and experi-
mental validations were conducted to analyze the differ-
ence between the overall applied strain on the sensor and
the localized tensile strain carried by the printed nano-
composite pattern embedded in the sensors. Detailed FEA
models and experimental validations of the FEA model
using a video extensometer were discussed in the Support-
ing Material. Numerical results showing the longitudinal
strain distribution in the substrate, nanocomposite pattern,
and the top PDMS layer at the 40% applied tensile strain
are depicted in Fig. 10f. The FEA simulation and experi-
mental results showed that the true tensile strain carried by
the printed nanocomposite was 6% smaller than the average
strain applied to the sensor during mechanical testing for
nanocomposite sensors with 1.5 wt% MWNT. Although this
smaller strain can increase the calculated GF of the strain
sensor, the difference in applied strain and actual strain on
the nanocomposite was so small that the correction factor
was not included in the experimental analysis to simplify the
data processing procedures.
In situ characterization of the piezoresistive sensing
mechanism
In situ micro-mechanical testing under SEM was conducted
to illustrate the piezoresistive sensing mechanism by dem-
onstrating the reorganization and rearrangement of MWNT
conductive network within the printed nanocomposite. The
SEM image of a relaxed nanocomposite sample (0% strain) is
shown in Fig. 11. Although only a low percentage of the
MWNTs was on the surface exposed to the SEM imaging,
the realignment of MWNT was visible in several zones. After
applying a 20% tensile strain on the sample, the rotation and
sliding of MWNT were observed, and is shown in the magni-
fied SEM images (P1–P5 zone) in Fig. 11. The zoomed SEM
images with solid borders show the initial orientation of the
MWNT (at 0% strain), while the pictures with dashed border
show the reorganization of MWNT network under 20% ten-
sile strain. The reduced gap between two adjacent nanotubes
can be seen in zones P1 and P3. Additionally, zones P2–P4
show two separated nanotubes connecting after applying
the load. The cumulative effect of the rearrangement of the
MWNTs in the conductive network resulted in the reduc-
tion of the resistance of the conductive nanocomposite by
13

Fig. 11  SEM images of the
working area in the in situ
micro-mechanical testing under
SEM: SEM images for five dif-
ferent zones (P1–P5) comparing
the initial unstrained state (show
in the boxes with solid borders)
and final loaded state at 20%
strain (show in boxes with
dashed borders)
increasing the tensile load. This piezoresistive sensing func-
tion of the strain sensor can be observed in Fig. 10c, d.
Human body motion recognition
To validate the application of the 3D-printed sensor as wear-
able sensors, a “smart” glove was prepared for human hand
motion detection. Five sensors were attached to each finger
on the glove to detect the finger motion, and one sensor was
attached to the wrist area to monitor the bending motion of
the wrist, as shown in Fig. 12a. Two tests were performed to
validate the sensors. First, the fingers and wrist were folded
and unfolded repeatedly, while the piezoresistive sensing
data were recorded simultaneously. Relative electrical resist-
ance changes between 22 and 55% were obtained during the
tests, as shown in Fig. 12b. In the second test, there were
10 s holding period after the bending and relaxation. The
recorded piezoresistive sensing results shown in Fig. 12c
were able to capture the bending and holding of each motion.
In particular, the plateau area in each cycle represented the
holding time in both the bending and relaxation periods of
the motion. The peaks of the plots showed the relaxation and
the valleys showed the bending motion. These experiments
demonstrated the potential of using the 3D-printed sensors
13
Applied Nanoscience
as wearable sensors, with potential applications in robotics
and biomedical sensors.
Conclusion
Piezoresistive strain sensors consisting of PDMS/MWNT
nanocomposites were 3D printed on a PDMS substrate and
characterized for potential wearable sensor applications. The
detailed nanocomposite formulation and 3D printing param-
eters were first optimized to obtain the sensors with the high-
est piezoresistive sensitivity. The strain sensing capability of
the sensors was evaluated by testing the printed sensors under
cyclic tensile loads. The experimental results showed that the
nanocomposites with an average GF of 13.01 in the 10–30%
strain range could be manufactured using a PDMS/MWNT
formulation with 1.5 wt% MWNTs, printed by 0.41 mm
diameter needles, and cured at 130 °C. The 3D printing pro-
cess was able to enhance the alignment of MWNTs in the
nanocomposites, leading to improved sensor performance.
The developed sensors with optimal properties carried up to
146% tensile strain before fracture, demonstrating their high
stretchability and flexibility. Experimental results showed
a linear sensing response, with an average GF of 12.15 in
the 10–70% strain range. Additionally, the highly repeatable
Applied Nanoscience

Fig. 12  a Smart glove demon-

strating the six possible individ-
ual sensing modes (five for the
fingers and one for the wrist);
b sensing response of repeated
bending of human hand joints;
c sensing response of hold and
bending of hand joints

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