Microelectronic Engineering 231 (2020) 111402

Contents lists available at ScienceDirect

Microelectronic Engineering
journal homepage: www.elsevier.com/locate/mee

Research paper

High-performance and wearable strain sensors based on graphene T

microfluidics and serpentine microchannels for human motion detection
⁎
Yang Liu , Jianze Huang, Guifu Ding, Zhuoqing Yang
National Key Laboratory of Science and Technology on Micro/Nano Fabrication, Shanghai Jiao Tong University, Shanghai 200240, PR China

A B S T R A C T

Inspired by microfluidics and microchannels, we demonstrate a new method based on graphene microfluidics and serpentine microchannels (GMSM) to fabricate and
pattern graphene/polymer composite film for pressure and strain measurement. With several types of experiment paraments including concentration of graphene
suspension, deposition frequency and width of microchannels, the resistance response of the sensors is measured as a function of mechanical stimulations. The
pressure sensor exhibits the high sensitivity (maximum: 0.27 /MPa) with ultrawide range (0–3 MPa), fast response and recovery time (88 ms, 217 ms), good
repeatability (250 cycles). For the strain sensor, high sensitivity (maximum: 60) with high deformation limits (75%), good repeatability (2000 cycles) have been
achieved. Finally, some human bio-signals are measured, demonstrated that the sensors have good potential for human-motions detecting and health surveillance.

1. Introduction effect owing to the coupling of nano fillers, such as tunnel resistance
between nanotubes [19,20], nano cracks' generation and disappearance
In recent years, flexible electronic tactile sensors are rapidly de- [21,22], relative motion between the nano-sized [23,24], and etc.
veloped for human health applications [1–3] such as motion detection Achieving high sensitivity, excellent stretchability, rapid response,
of limbs, wrist pulse detection, blood pressure measurement, and linearity, cyclic stability, bio-compatibility requires innovative ap-
speech recognition. With the capability to translate external physical proaches [25–27]. Alternative microstructures such as micro/nano
stimulation to visible electrical signals, tactile sensors have application porous structures [28,29], micro-pyramid arrays from anisotropic
prospects in fields of clinical diagnosis [4], health monitoring [5], etching [30,31], serpentine and wavy pattern [32,33], rough substrate
flexible electronic skin [6], human/machine interfaces [7] and so on. by replica moulding [34,35] are designed. However, these manufacture
Generally, tactile sensors are based on piezoresistive effect, capacitance methods adopted are multistep, expensive, bio-toxicity and environ-
effect and piezoelectric effect [8,9]. ment unfriendly. Therefore, superior methods are desired to satisfy
Resistance of the tactile sensors changes with pressure or strain both reliable performance and economic fabrication process. Multilayer
applying based on piezoresistive effect. Tactile sensors based on pie- graphene nanoflakes have excellent capacity of mechanical property,
zoresistivity are widely reported due to short period, good feasibility chemical stability, and it has potential for commodity manufacturing.
and wide sensing range [10,11]. Pressure sensors based on crystalline Si And graphene is widely used as active materials for tactile sensing
[12] and metallic strain sensors [13], as kinds of traditional tactile [36,37]. 3D printing technology is an efficient method to fabricate and
sensors, have been developed for commercial purposes. Recently, along pattern flexible polymer compared with dry etching and photo-
with the development of nano materials and polymer elastomers, un- lithography based on SU8 negative photoresist [38]. Various micro-
conventional preparation methods have been chosen to fabricate high- structures can be fabricated through moulding and demoulding pro-
performance tactile sensors. Commonly, graphene nanoflakes [14], cesses based on 3D-prinetd technology, for example microchannels.
carbon nanotubes [15], metal nanowires [16] and graphite nano- Liquid-filled tactile sensors based on microchannels and microfluids
particles [17] are deposited on flexible substrates to prepare conductive have been reported, with good stretchability and high performance
and stretchable pathways/networks. The contact resistances between [39–41].
sensing elements and electrodes are analyzed when pressure or stress is In our previous work [42], pressure sensors based on GMSM were
applied, which can result in the change of electrical property. Beyond prepared. In this paper, based on graphene microfluidics and serpentine
that, nanomaterials mentioned above are embedded in polymer elas- microchannels, we demonstrate a new method to fabricate and pattern
tomers to construct conductive composites, which can form conductive graphene/polymer composite film for pressure and strain monitoring.
electricity pathways [18]. Composites exhibit significant piezoresistive Herein, a condensed physical model is established, and the resistance

⁎
Corresponding author.
E-mail address: [email protected] (Y. Liu).

https://doi.org/10.1016/j.mee.2020.111402
Received 25 February 2020; Received in revised form 17 June 2020; Accepted 14 July 2020
Available online 21 July 2020
0167-9317/ © 2020 Elsevier B.V. All rights reserved.
Y. Liu, et al. Microelectronic Engineering 231 (2020) 111402

responding mechanism is analyzed quantitatively. The calculation same time. The cyclic pressure and strain were both applied by a uni-
method of pressure sensor is optimized and performance testing is versal testing machine (ZwickRoell, Z020).
further perfected. As well, the preparation and properties character-
ization of strain sensors are realized. Finally, human bio-signals of wrist 3. Results and discussion
pulse wave, finger and wrist bend, finger pressing, plantar pressure are
measured, and the results demonstrate that the GMSM sensors have 3.1. Morphology and sensing mechanism
capability for human-motions detecting and health monitor. Several
technologies for the wearable strain sensor are advanced: (i) used for Nano/micro porous graphene structure is generated owing to gra-
not only pressure sensing but strain sensing based on GMSM; (ii) high phene nanoflakes depositing layer after layer. As the SEM photos shown
sensitivity (0.27 /MPa for pressure sensing and 60 for strain sensing) in Fig. 2a, it can be noticed that graphene nanoflakes are embedded into
and wide measurement range(0–3 MPa for pressure sensing and 75% polymer with good adhesion and dispersibility. Some nano/micro-pores
for strain sensing; (iii) application for detecting human not just large remain inspite of the protective layer penetrating into multilayer gra-
motions (finger pressing, bending, writing and foot treading) more than phene nanoflakes, as shown in Fig. 2b-d. The resistance of graphene/
slight movement (pulse wave, swallowing and speaking); (iv) based on polymer composite layer covers two aspects Rcomposite and Rnanopore. (1)
efficient, eco-friendly and bio-friendly process technology compared Rcomposite originates from three parts, respectively, inherent resistance
with conventional processes. of graphene, contact resistance between nanoflakes, and inter-flake
tunnel resistance (Fig. 2e). The intrinsic resistance can be regard as
2. Experimental constant and ignored, because graphene has ultrahigh intrinsic carrier
mobility and unremarkable piezoresistive effect. When the inter-dis-
2.1. Preparation of graphene/deionized water suspension tance is short enough that ultrathin polymer exists between neigh-
bouring nanoflakes, tunnelling phenomena proceeds and local re-
Reduced graphene oxide (RGO, TNPRGO, Chengdu Organic sistance varies with loading. (2) The Rnanopore consists of the inherent
Chemicals Co. Ltd.) and deionized water were mixed thoroughly at resistance of graphene which is ignored before and the contact re-
30 °C for 6 h. It is worth mentioning that RGO occurrs as water-in- sistance between the normal and radial distributions of graphene na-
soluble substance. But dispersibility of RGO can be efficiently solved by noflakes. The equivalent circuit is shown in Fig. 2f, and Rnanopore can be
the addition of surfactant. The effective constituent of surfactant is expressed as.
sodium dodecyl benzene sulfonate (SDBS, TNWDIS, Chengdu Organic for pressure applied:
Chemicals Co. Ltd., 30% weight of graphene). Accordingly, graphene
nanoflakes flew through the entire microchannels and deposited uni- Rnanopore |=[RrI & nI + (RnI & nII + RrII & nII ) RnI & rII ]
formly as shown in fig. S1. [RrI & nII + (RnI & nII RnI & rII ) RrII & nII ]
RrI & rII
2.2. Fabrication of pressure sensors and strain sensors for strain applied:

The fabrication process is shown in Fig. 1, which also is described in Rnanopore |=[RrI & nI + (RrI & rII + RrII & nII ) RrI & nII ]
our previous work. [RnI & rII + (RrI & rII RrI & nII ) RrII & nII ]
RnI & nII
2.3. Characterization
Nanopore is suffered intense deformation during loading, resulting
The micromophology of the composite layers of the sensors was in the decrease/increase of overlapping areas of nanoflakes in normal/
studied by a field emission SEM (ZEISS, Ultra55). The performance radial directions. Composite materials with nanopores have lower
measurement system designed for resistance response test are shown in Young's modulus, which signifies that obvious change of Rnanopore
fig. S2 a-b. Pressure was applied by a bonding tester (RHESCA, PTR- trends to present under low pressure or stress.
1101). Strain was applied by a self-made test system including a 5-
phase stepping motor (Orientalmotor), a 2-Axis stage controller (CHUO 3.2. GMSM for pressure sensing
SEIKI, QT-CM2–35), a force sensor (Honeywell, SC500), a microscope
and a custom-made 3-Axis translation stage. A digital multimeter Concentrations of graphene suspension and deposition frequency
(Keysight 34465A) was used to measure the change of resistance at the are significant variables in the resistance response of the GMSM pres-
sure sensor. The relative resistance-pressure curves of the flexible
pressure sensor under different concentrations of graphene suspension
are shown in Fig. 3a. The ΔR/R0 increases obviously with the con-
centrations (from 0.3 mg/ml to 5 mg/ml) of graphene suspension in-
creasing at deposition frequency for 5 times. As shown in Fig. 3b, when
the graphene suspension concentration is 5 mg/ml, along with different
graphene deposition frequency from 2 times to 5 times, the ΔR/R0
changes more and more rapidly with pressure. The sensitivity rises
along with concentrations of graphene suspension and deposition fre-
quency increasing. The highest sensitivity is observed with 5 mg/ml
graphene suspension and deposition frequency for 5 times. The sensi-
tivity can be defined as δ(ΔR/R0)/δP, where δ(ΔR/R0) refers to the
change of relative resistance, and δP is the change of pressure. The
sensitivity of 5-layers sensor with 5 mg/ml is not lower than 0.20 /MPa
and reaches a maximum 0.27 /MPa at ~1 MPa. The pressure sensing
capability is remarked up to 3 MPa.
The force-displacement behavior of the GMSM pressure sensor is
Fig. 1. Main fabrication process of the flexible sensor and flexibility feature of showed in Fig. 3c. It can be noticed that the compressing course ex-
pressure sensor and strain sensor. hibits two obvious regions. In small pressure range (region I, 0– 1 MPa),

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Y. Liu, et al. Microelectronic Engineering 231 (2020) 111402

Fig. 2. SEM photo of nano/micro porous graphene structure and the components of resistance. (a)Vertical view of the surface: grapheme nanoflakes embedded into
PDMS; (b)Cross-sectional SEM photos of the grapheme/PDMS composite layer: many nanopores remain and form porous structure; (c-d)Higher magnification view of
the composite layer; (e) The origination of RComposite including inherent resistance of graphene, contact resistance between nanoflakes, and inter-flake tunnel
resistance; (f) The definition of Rnanopore: inter-graphene contact resistance of overlap region in the nano-pore spaces.

chiefly contribution to resistance changing comes from the change of stress directly causes the decrease of contact resistance and tunnel re-
Rnanopore, which varies significantly under nanopore collapsing. The sistance. Totally, the Rcomposite slowly increases and the sensitivity de-
contact resistance in radial/normal direction decreases/increases. creases. Concentrations of graphene suspension and deposition fre-
Graphene nanoflakes in normal direction (RnI&nII→∞) are insulated, quency are direct acting factors for quantity of nanopores, therefore
and Rnanopore can be expressed as multi-depositional pressure sensor with high concentration graphene
suspension shows high sensitivity. But with too high concentrations of
Rnanopore = [RrI & nI + (RnI & rII ] graphene suspension, the capillary between graphene nanoflakes pro-
[RrI & nII + (RrI & nII duce large negative pressure, resulting in volume contraction during
RrI & rII thermal treatment. With low intensity of graphene before condensation,
significant plastic cracks appear. As the increase of deposition fre-
With further collapse of nanopores, the contact resistance between quency, graphene nanoflakes continually attaches on the sidewalls and
graphene nanoflakes increases until insulates with others(RrI&nI, RnI&rII, bottom of microchannels, which causes the increase of frictional drag.
RrII&nII, RrI&nII→∞), and Rnanopore ≈RrI&rII. This may be the reason why Microfluids cannot flow through the entire microchannels when de-
the sensitivity increases in region I. Although RrI&rII decreases under position for more times.
pressure applied, the increase of contact resistance in normal direction Besides, the response and recovery time are measured under a 50 g
is more significant. weight as shown in previous work and fig. S3. The response time and
In the second region (1– 3 MPa), nanopores are compacted, re- recovery time are 88 ms and 217 ms respectively. Recovery time delay
sulting in the pressure rapidly increasing with displacement. In this exists in this GMSM pressure sensor because of viscoelasticity and creep
region II, Rnanopore is approximately a constant, and the change of recovery of polymers. Moreover, cyclic stability is examined for cap-
Rcomposite is the dominant factor to influence resistance variation. Shear ability assessment of dynamic performance. As shown in fig. S4, the
stress brings about the dislocation of graphene nanoflakes or cut-off of repeatability is tested under 250 cycles, and the GMSM pressure sensor
tunnel effect, and local resistance increases. However, compressive demonstrates good stability. The results show that the nanopores inside

Fig. 3. (a)Resistance response (ΔR/R0) vs. applied pressure at different concentrations of grapheme suspension (0.3, 1, 3, 5 mg/ml) and 5-times depositions; (b) ΔR/
R0 changes with pressure at different numbers of deposition frequency (2–5 times) with 5 mg/ml grapheme suspension; (c) The force-displacement behavior of the
pressure sensor(right: force condition of nanopore with pressure applying).

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Y. Liu, et al. Microelectronic Engineering 231 (2020) 111402

Fig. 4. (a) Resistance response (ΔR/R0) vs. applied strain with different width of microchannels(500 μm,700 μm, or 1 mm); (b) the simulation result of tensile test.
The stress of different microchannel widths when strain is applied from 10% to 70%; (c) Repeatability test of the pressure sensor for 2000 cycles. The change of R0 is
shown in the top of image.

still remain at repeated pressure loading, and the GMSM pressure As shown in Fig. 4c, the repeatability test under 2000 cycles of 30%
sensors can operate under dynamic pressure. strain is conducted at a time cycle of 3 s, and the GMSM strain sensor
demonstrates good cyclic stability and repeatability. The initial re-
sistance R0 decreases about 4% after 2000 cycles, indicating that the
3.3. GMSM for strain sensing
GMSM strain sensor remains stable during the experiment.
Resistance response (ΔR/R0) vs. applied strain is compared for dif-
ferent width of microchannels (500 μm, 700 μm, or 1 mm) as shown in 3.4. GMSM strain sensor for human motion detections
Fig. 4a. Graphene suspension under equal volume and concentration is
dropped into serpentine microchannels with different sizes. The wider With a view to detecting human motions and monitor human
microchannel is, the more rapidly the ΔR/R0 changes with strain ap- health, the sensors proposed here show excellent characteristics of high
plying. With microchannel width increasing, the sensitivity will im- sensitivity, wide measurement range, quick response, and cycling sta-
prove. The GMSM strain sensor based on 1 mm microchannels shows bility. On the one hand, serious fluctuation in human motion can be
high sensitivity level. Similarly, the sensitivity of the GMSM strain detected efficiently. Fig. 5a-b show the resistance response curve of the
sensor can be expressed as δ(ΔR/R0)/δ(ΔL/L0), where δ(ΔR/R0) is the GMSM pressure sensor for finger pressing and foot treading. These re-
change of relative resistance, and δ(ΔL/L0) is the change of strain. The sults illustrate the pressure sensing capability of wide-range applica-
experimental results express that the ΔR/R0 vs. strain curves can be tions. The GMSM strain sensor was attached to finger joint of tester to
divided into two phases: (i)increasing sensitivity (no less than 10) for monitor finger bending movements. The measurement results of human
small deformation (< 45%). (ii) stable sensitivity (60) for large de- index finger bending are displayed in Fig. 5c. What's more, excellent
formation (45% - 75%). This GMSM strain sensor with high sensitivity recovery performance is shown after undergoing a finger bending cycle.
and wide range are better than previously reported ([43–49], Table S1). The GMSM strain sensor was fixed to tester's right thumb to measure
For small elongation, both stretching in normal direction and bending process of finger when writing. The tester wrote the Chinese
compressing in radial direction of nanopores lead to the relative characters “Shang Hai”. The resistance response is exhibited in Fig. 5d.
movement of graphene nanoflakes, which is the major contribution to The first half of the curve is “Shang”, and the second half is “Hai”.
Rnanopore changing. The contact resistance in normal direction increases Combining with machine learning technology and artificial intelligence
to insulation (RnI&nII→∞), and Rnanopore can be simplified as technology, it has a potential application in handwriting recognition.
Rnanopore |=[RrI & nI + (RrI & rII + RrII & nII ) RrI & nII ] On the one hand, the sensors can be used for slight movement de-
[RnI & rII + (RrI & rII RrI & nII ) RrII & nII ] tecting in human body significantly. The GMSM strain sensor was held
With external strain applied, the contact resistance between gra- in tester's wrist by medical adhesive tape. The pulse waveform of tester
phene nanoflakes in normal and radial direction (RrI&nI, RnI&rII, RrII&nII, is shown in Fig. 5e. The heart rate is about 84 times/min and within
RrI&nII) increases until disconnects with each other. The sensitivity normal range. Furthermore, three typical pulse peaks, which are per-
continuously increases when deformation is less than 45%. For large cussion wave, tidal wave and dicrotic wave, can be identified distinctly.
deformation, there is almost zero radial distance in nanopores because The time delay between percussion wave and tidal wave (ΔtDVP) and
of the ultimate deformation, but sliding and misalignment between the radial augmentation index (AIr) are analyzed, which are 0.10 s and
adjacent nanoflakes still play a role. Due to contact separation of 0.64 respectively. And the parameters are normal to a 24-year-old
complete connection nanoflakes and decrease of tunnel current under tester. Fig. 5f-g shows that throat muscles movements and vocal cord
strain, both contact resistance between nanoflakes and inter-flake vibration. When tester was swallowing, GMSM strain sensor fixed in
tunnel resistance will increase, leading to the change of Rcomposite. With throat was subject to tensile stress. When tester said different words
strain applying, distance between neighbouring nanoflakes will in- “Hello”, “World”, the GMSM strain sensor exhibited good sensitivity.
crease until cut-off distance, at which nanoflakes are isolated and no Different words correspond to different curves. With each word re-
current flow through adjacent nanoflakes. Thereby Rcomposite will in- peated 4 times, the curves of identical word are approximately the
crease rapidly. Stress effect and the amount of graphene per unit vo- same. These experimental results indicate that the GMSM strain sensor
lume are main aspects of the influence of microchannel width. The has good potential application for voice recognition.
stress on the microchannel increases obviously as the applied strain
increasing, and wider microchannel shows advantage. Stress level is 4. Conclusions
comparatively higher in wider microchannel as shown in the simulation
result (Fig. 4b). With 1 mm microchannels, more stress concentrates In summary, based on microfluidics and microchannels, we de-
during tension test, leading to higher sensitivity. Beyond that, there is a monstrate a new method to fabricate and pattern graphene/polymer
lower concentration graphene nanoflakes in the wider microchannels, composite film for pressure and strain monitoring and a condensed
in which graphene conductive pathway is more likely to be isolated. model to quantitatively analyze the resistance response mechanism.

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Y. Liu, et al. Microelectronic Engineering 231 (2020) 111402

Fig. 5. Applications for human motion detection and healthcare. (a)The resistance response curve of finger pressing; (b) the resistance response curve of foot
treading; (c)Measurement result of human index finger multiple bending and bending with different angles; (d)The resistance response of strain sensor fixed to
tester's right thumb, when writing the chinese characters of “Shang Hai”; (e)Pulse wave of a 24-year-old tester, the inset is the magnified view of the waveform
marked; (f) Resistance changing of tester ‘s swallowing; (g) Resistance response when tester speaks different words.

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