Stable Wearable Strain Sensors on Textiles by Direct Laser Writing of Graphene Wen Liu 1,2 , Yihe Huang 2 , Yudong Peng 1,2 , Monik Walczak 3 , Dongwang 1 , Qian Chen 1 , Zhu Liu 1,2* and Lin Li 2 1 Department of Materials, Faculty of Science and Engineering, The University of Manchester, Oxford Road, Manchester M13 9PL, UK 2 Laser Processing Research Centre, Department of Mechanical, Aerospace and Civil Engineering, Faculty of Science and Engineering, The University of Manchester, Manchester, M13 9PL, UK 3 Department of Chemistry, Faculty of Science and Engineering, The University of Manchester, Oxford Road, Manchester M13 9PL, UK *Corresponding author: [email protected]1
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Research Explorer | The University of Manchester · Web viewTo start, basic mechanical properties and electrical properties were investigated to evaluate the sensor’s limitation.
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intensity ratio of LIG with increasing laser fluence.
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Figure 6. Raman mapping of (a) d/g peak intensity ratio (d) 2d/g peak intensity ratio; (c,d) TEM
image of LIG obtained at 20.5mJ/cm2.
The synthesizeds of LIG based on the PI fabric was studied with by X-ray photoelectron
spectroscopy (XPS). Figure 7a compares the chemical composition of PI fabric and LIG,
showing the significant suppression of O and N elements after laser scribing. The peaks of Si2s
and Si2p also disappeared in the XPS survey of LIG, which may be related to the surface dust
removed by laser cleaning. This comparison might suggest that the decreased O and N elements
emitted from the surface of the PI fabric, in the form of gas oxidation, causing the porous
structure of LIG which can be observed in the SEM images. Rice University has investigated the
mechanism of the conversion of PI films to LIG using a long wavelength CO2 laser42. They
suggested that high localised temperature at least of 2500 ˚C was is required to break the C-O
and C-N bonds. These oxygen and nitrogen atoms would will then rearrange and form gases. In
our work, using a UV laser (355 nm wavelength), photon energy of 3.59 ev is enough to achieve
the breakage of these bonds through a the photochemical process without a high temperature34.
For the left remaining carbon atoms, a the graphitization process can be triggered through
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thermal dynamic effects. They also found that specific structure features including aromatic and
imide repeat units were are essential to generalize this laser-induced graphitization process49.
High resolution of C1s XPS spectraums of PI fabric and LIG, as illustrated in figure 7b,
indicate that C-O-C, C-N and C=O bonds are significantly decreased by the laser ablation. This
means that the Sp2 carbons dominate the composition of LIG50. Figure 7c shows the high
resolution of O1s XPS spectraums which consists of C-O and C=O bonds. It can be seen that
majority of C-O bonds were are converted into C=O bonds which have higher binding energy
during the laser process. The reduceion of C-N bonds also can also be observed in figure 7d.
Figure 7. XPS characterization of PI fabric and LIG. (a) XPS surveys of the PI fabric and LIG;
(b) High resolution C1s XPS spectrum of the PI fabric and LIG; (c) High resolution O1s XPS
spectrum of the PI fabric and LIG; (d) High resolution N1s XPS spectrum of the PI fabric and
LIG.
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3.3 Performance analyses of LIG fabric strain sensor.
The electromechanical performance of the LIG fabric sensor was comprehensively studied by
continuously recording the resistance change while the sensor was stretched. To start, basic
mechanical properties and electrical properties were investigated to evaluate the sensor’s
limitation. In figure 8a and 8b, a tension-recovery cycle of the PI fabric in parallel and diagonal
directions are shown. The inserted illustrations show the difference in the woven direction of the
PI fabric. It is clear that in the parallel direction, the PI fabric cannot recover after stretching
even under subtle strains. However, the fabric exhibited good recovery in the diagonal direction
within a certain range which means that it is possible to assembly sensors in this direction. The
anisotropy of the stretchability of the fabric was due to the different mutual tension and friction
in different directions after weaving51. In general, the weaving method endows the non-elastic PI
fabric with stretch-recovery ability within a small strain range. Figure 8c shows a primary
tensile stress/strain curve of the PI fabric. Under strain up to 14%, the plot stays good linearity
below 4% strain, representing 4% elastic range whereas plastic deformation occurreds above this
value. The excellent electrical conductivity of LIG was also found through a 4-wire resistance
test which is shown in figure 8d. The sheet resistance can be as low as 20 /sq when the laser
fluence was 22 mJ/cm2. Futher increase in laser fluence began to partially burn out the fabric
without noticeable reduction on sheet resistance.
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Figure 8. Tensile stress/strain curve of PI fabric (a) in parallel direction; (b) in diagonal
direction; (d) Tensile stress/strain curve of PI fabric (14% strain); (c) Sheet resistance of LIG
with various laser fluence.
In this study, the sensitivity, strain threshold, repeatability and response to different strain and
strain rate were examined by sensors fabricated at 20.5 mJ/cm2 of laser fluence. In fact, laser
fluence was considered to be the most relevant factor affecting sensitivity when regarding to the
laser-prepared active materials for strain sensors. The electrical properties of LIG are dominated
by the crystallization quality and defects during laser processing, which has been fully studied by
previous researches14. The LIG with better electrical properties will be more sensitive to minor
change in external strain. The curves of the resistance change versus strain of sensors
synthesized with different laser fluence are shown in figure S5, which explains this relationship
between the quality of LIG and the sensitivity of the LIG fabric sensor. In addition, it is worth
mentioning that the laser fluence may also affect the sensitivity of this fabric sensor by refining
the size of carbon particles grown on the edges of fibers. Figure S6 (An x15000-magnified SEM
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photo) proves that nano-sized carbon particles can be generated by controlling the laser fluence
without damaging the substrate. This will lead to a significant increase of the contacting and
overlapping areas among carbon particles, which may amplify the strain change and contribute to
the high sensitivity.
As shown in figure 9a, the sensor with a rectangle pattern (30 mm x 10 mm) shows a linear
response up to 4% strain elongation. To characterize the sensitivity of the sensor, the gauge
factor (GF) can be calculated on average as 21.4 (GF max=27) through the equation (1).
Although this value is inferior to some previously reported strain sensors which used elastomer
polymer as substrates, such as a laser-carbonized PDMS strain sensor reported by Rehim14 with a
GF up to 20000, a graphene-coated strain sensor based on glass fabric/silicone composite with a
GF up to 11352 and a graphene-on-polymer strain sensor which can reach GF up to 100053. This
large-area fabric-based LIG strain sensor owns a numbers of advantages, including low detection
limitation, high stability, a simple fabrication procedure technique and etc. On the other hand, the
sensitivity of this LIG fabric strain sensor is still competitive compared to conventional fabric-
based strain sensors. The reason is that the traditional fabric strain sensor cannot achieve large
sensing area through coating or deposition methods. Table S2 listsed a the comparison of
fabrication details and performance with various recent fabric strain sensors.
Basically, the mechanism of strain sensors can be grouped into two catalogues: one is the crack-
controlled design which depends on the destruction and recovery of the structure during the
stretching process54. The other one is the change in the number of carrier channels which is
caused by the variation of the contact area of the active materials55. Figure S7 show illustrates the
SEM images of the fiber surface morphology in two different directions under stretching. Based
on the mechanism of strain sensors, the stretching and recovery properties of the strain sensor
can be considered to mainly depend on the relatively stable 3D network structure of active
materials during stretching. The choice of the substrate weaving direction (diagonal direction)
directly determines the stretching range of the fabric strain sensor. On the other hand, the loss of
electrical properties during the stretching cyclse can be attributed to the partial detachment of the
active particles at the edge of the fiber. The zoom-in graph of the resistance change response
within the strain range of 0.1%, as plotted in Figure 9b, represents the small detection limitation
of strain which can be as low as 0.08%. This may be due to the carbon nanoparticles grown on
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the fibre framework which are observed in SEM graphs. An ultra-small particle size indicatesed
that a weak strain can also cause a sufficient amount of active material to be separated from each
other, producing a resolvable resistance response. Further evidence is shown in figure S8, in
which all the plots show similar threshould values around 0.08% under different strain at 1%,
2%, 3% and 4% respectively. Figure 9c shows the acquisition of stable signals of the sensor
device under various strain loads. It is clear that the change of resistance increases with the
growth of applied strain in an approximately linear law. In figure 9d, it can be seen that the
amplitude of signals under different strain loading rate remain consistent for several loading and
unloading cycles. Applying repeated external load, cracks in the fiber skeleton initiate, propagate
and recover, dominating the change in electrical properties. Below the elastic deformation scale,
the peak value and the bottom value of the resistance signals were are maintained within a
relatively stable range. This presents a the good signal recording performance of the fabric strain
sensor without obvious lag errors. The cycle test is depicted in figure 9e to examine mechanical
durability. It can be found that only 4% deviation is generated after 1000 cycles at ε=4%. This
means that there is around 4% of the resistance change loss after 1000 loading-unloading
cycles.There is also a difference of the normalized resistance change between the statical and
dynamical test, which is caused by patially electrical properites loss during long-term loading
and unloading process. The zoom-in curve of 4 cycles is compared with the strain cycles in
figure 9f, exhibiting small lag errors of 250 ms during long-term loading and unloading cycles.
The fatigue test of the PI fabric can be shown in figure S9 to indicate the stability of the PI fabric
substrate.
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Figure 9. (a)The resistance change versus strain plot within the strain range of 4%; (b) Zoom-in
figure a within the strain range of 0.1%; (c) response of resistance change under different strain
value; (d) response of resistance change under different strain rate at 2% strain; (e) cycle test at
4% strain for 1000 cycles; (f) Zoomed in figure of resistance change cycles comparing to the
strain cycles. (sensors for this experimental part were fabricated at a laser fluence of 20.5
mJ/cm2).
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Figure 10. Photographs showing the LIG fabric strain sensor in human motion detection. (a) The
sensor applied to the knuckle of the index finger, examing finger bending; (b) The sensor
attached to the wrist joint to detect wrist flexion; (c) The sensor attached to the bicipital muscle
to record the movement of the muscle.
3.4 Applications of LIG fabric strain sensors on human motion.
Experiments of practical response to different human motions were carried out to explore the
utility of this LIG fabric strain sensor. Devices used in this section were fabricated at a laser
fluence of 20.5 mJ/cm2 due to the highest sensitivity. Finger bending was firstly detected, as
shown in figure 10a, for 9 bending-stretching cycles. cliff-shaped peaks for each cycle were
derived from the nonlinear change of joint bending angle. Figure 10b demonstrates the resistance
change of the sensor in response to the flexion of the wrist. The steepness of signal peak in this
curve is slightly larger than the plot of finger bending, resulting from the larger separation of the
wrist joint. When the LIG strain sensor was attached on the bicipital muscle which is shown in
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figure 10c, the movements of this muscle were recorded in detail. At the top of each peak,
fluctuation of the curve can be observed which is due to the slight muscle twitch in the tense
state. The results above further prove the potential applications of the LIG fabric strain sensors to
distinguish various signals of human motion.
4. Conclusion
We have demonstrated a UV laser direct writing technique for the production of porous graphene
strain sensors directly on PI fabrics. The results demonstrated that the formation of LIG is
strongly controlled by the laser fluence, which further influencesd the sensing performance of
assembled LIG sensors. This LIG device has a low sheet resistance of 20 /sq, a maximum GF
of 27, a small strain threshold value of 0.08% and high mechanical stability of 4 % resistance
change loss after 1000 cycles. Through this sensor, various human motion signals were detected
and recorded in the form of resistance change, indicating the promising potential applications in
the health monitoring on smart wearables.
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