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Fabricating a highly sensitive graphene

nanoplatelets resistance-based
temperature sensor
Mohammed Gamil
Department of Mechanical Engineering, Faculty of Engineering at Shoubra, Benha University Cairo, Egypt
Nagih M. Shaalan
Department of Physics, College of Science, King Faisal University, Al-Ahsa, Saudi Arabia and
Physics Department, Faculty of Science, Assiut University, Assiut, Egypt, and
Ahmed Abd El-Moneim
Graphene Center of Excellence for Energy and Electronic Applications, Egypt-Japan University of Science and Technology,
New Borg El-Arab City, Egypt

Abstract
Purpose – This study aims to present an efficient and reliable graphene nanoplatelets (GNPs)-based temperature sensor.
Design/methodology/approach – A high-quality dispersion of GNPs was dropped by casting method on platinum electrodes deposited on a
polyethylene terephthalate (PET) substrate. The GNPs were characterized by scanning electron microscope, Raman spectroscopy and X-ray
diffraction spectra to ensure its purity and quality. The temperature sensing behavior of the fabricated sensor was examined by subjecting it to
different temperatures, range from room temperature (RT) to 150 °C.
Findings – Excellent resistance linearity with temperature change was achieved. Temperature coefficient of resistance of the fabricated sensor was
calculated as 1.4  10–3°C. The sensor also showed excellent repeatability and stability for the measured temperature range. Good response and
recovery times were evaluated at all the measured temperatures. With measuring the sensor response, the ambient temperature can be determined.
Originality/value – The present work presents a new simply and low cost fabricated temperature sensor based on GNPs working at a wide
temperature range.
Keywords Graphene nanoplatelets, Temperature sensor, Resistance-base sensor, Thin film sensors
Paper type Research paper

1. Introduction that are identical to those found in the walls of carbon


nanotubes, but in a planar form. The unique size and platelet
Temperature sensing is very important for various engineering morphology of GNPs makes it effective at providing barrier
applications. Easy-fabrication, low-cost and reliable properties, while its pure graphitic composition makes it as
temperature sensors are desired for these applications. In the
excellent electrical and thermal conductors (Kuan et al., 2018;
last few years there has been a growing interest in using
Gamil et al., 2014b; Gamil et al., 2012; Gamil et al., 2013). As a
graphene as a resistance base temperature sensor due to its
result, GNPs are considered a game changer for numerous
superior physical properties (Wang et al., 2010; Bolotin et al.,
sensing application. Recently, GNPs have aroused tremendous
2008; Novoselov et al., 2007; Schedin et al., 2007; Ghosh et al.,
interest for various sensing applications (Gamil et al., 2014a;
2008). Graphene is the thinnest known material that gathers a
Gamil et al., 2014c; Sayed et al., 2016; Sayed et al., 2015).
lot of interest after its discovery by Novoselov et al. due to its
However, there are only few reports on using GNPs as a
superior mechanical and physical properties (Novoselov et al.,
temperature-based resistance sensor.
2004). Graphene is a single layer of carbon atoms placed in a
Yang et al. (2015) fabricated a wearable temperature sensor
honey comb lattice structure.
from graphene nano-walls (GNWs) over a
GNPs are stacks of multigraphene layers in a two-
polydimethylsiloxane substrate. But it only exhibited a small
dimensional nano particulate format (basal planes of carbon
atoms packed into a hexagonal array) having a platelet shape dynamic range (35 to 45°C). In addition, vast edges and defects

The authors gratefully acknowledge the generous technical and financial


support of Benha University, Assiut University and Egypt-Japan University
The current issue and full text archive of this journal is available on Emerald
of Science and Technology (E-JUST).
Insight at: https://www.emerald.com/insight/0260-2288.htm
Conflict of interest. On behalf of all authors, the corresponding author states
that there is no conflict of interest.
Sensor Review
41/3 (2021) 251–259 Received 19 January 2021
© Emerald Publishing Limited [ISSN 0260-2288] Revised 17 March 2021
[DOI 10.1108/SR-01-2021-0023] Accepted 9 April 2021

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were existed in the prepared GNWs. Sahoo et al. (2012) Figure 1 Fabrication processes of the graphene-based temperature
succeeded to fabricate an ultra-fast graphene based sensor on PET substrate
temperature sensor. The sensor was prepared by drop casting
the graphene oxide (GO) prepared by the modified hummer
method (Hummers and Offeman, 1958) on a platinum
interdigital electrodes (Pt-IDE). The GO is reduced by hydrazine (a) (b)
vapor. The sensor is then characterized to ensure it sensitivity. It
was found that its sensitivity is much better than the platinum
thermo sensor. However, the quality of the reduced GO is very
low due to the high intensity of the D peak which is related to the
(c) (d)
number of defects with respect to the G peak in the Raman
spectroscopy. Moreover, the maximum measured temperature Notes: (a) PET substrate; (b) Pt deposition; (c) Wire bonding;
doesn’t exceed 127°C. In addition, the fabricated sensor can’t be (d) GNPs drop casting
commercialized in its fabricated form.
Davaji et al. (2017) fabricated graphene based resistance
1 mm gap. Wire bonding is then made to provide the necessary
sensors on different substrates by microfabrication technology. A
connecting terminals as shown in Figure 1(c). Finally, an average
single layer graphene was deposited on copper foil by chemical
volume of 5 mm3 of the GNPs suspension is drop casted on the
vapor deposition (CVD) and then transferred to a silicon dioxide
gap and left for 1 h to dry as shown in Figure 1(d). A film of
(SiO2)/Si substrate as well as a silicon nitride (SiN) membrane
GNPs with 1 m m average thickness is formed between the two
(Fu et al., 2017). The fabricated temperature sensors were
electrodes. Figure 2(a) shows the actual image for the fabricated
subjected to different temperatures and their responses were
sensor before GNPs deposition meanwhile Figure 2(b) shows the
measured simultaneously. It was found that the SiN membrane
graphene-based resistance sensor in its final form after the
shows the highest sensitivity if it is compared with the (SiO2)/Si deposition of GNPs by drop casting. The fabricated sensor has a
substrate. Sensor fabrication is hard due to the graphene square area of 14  15 mm2, including the PET and pads. We
preparation by CVD and the transfer method to the substrates. fabricated the sensor on a flexible substrate to accommodate
Sahatiya et al. (2016) fabricated a wearable temperature flexible applications such as flexible electronics. Figure 2(c)
sensor from Solare exfoliated reduced graphene oxide (SrGO) shows real image for the fabricated sensor subjected to bending
with high sensitivity. A flexible polyimide substrate was used to stress. It can be seen that the GNPs film provides good adhesion
deposit the SrGO. Ultra-sensitive wearable human body with the PET substrate. Moreover, there is no cracking or pealing
temperature sensing is achieved in the temperature range of up for the film after several bending cycles.
35°C to 45°C. The measured temperature range of this
fabricated temperature sensor is small and not suitable for 2.3 Sensor characterizations
higher temperatures measurements. The fabricated graphene-based temperature sensor was
In the present study, a highly sensitive graphene-based characterized by the test setup shown in Figure 3. The test
temperature sensor is fabricated by drop casting a high-quality setup consists mainly of a testing chamber (Quartz tube) that
suspension of GNPs over platinum electrodes deposited on a can be heated by an electric furnace. The heating temperature
flexible polyethylene terephthalate (PET) substrate. A simple, inside the testing chamber is controlled by a commercial
easy and low-cost fabrication technique is presented for the temperature control unit. The fabricated sensor is introduced
current temperature sensor. Furthermore, a wider range of to the chamber that was previously heated to the desired
temperature sensing is achieved. The fabricated sensor justifies measured temperature. The sensor was carried on transverse
the use of GNPs for device fabrication. The GNPs was lab-made system. The sensor was pushed inside the furnace for
characterized by X-ray diffraction (XRD), scanning electron getting its steady response, and then it was rapidly pulled out to
microscope (SEM) and Raman spectroscopy techniques. the room temperature (RT). The output signals measured from
the fabricated sensor are transferred directly to a data
2. Experimental procedures acquisition unit (Multi-channel LXI Agilent 34972 A), which is
connect directly to the PC for recording the signal. The furnace
2.1 Graphene nanoplatelets characterization
temperature was changed from RT up to 150°C.
Ultra-high concentration dispersion of GNPs were supplied by
Graphene Laboratories Inc. (760 Koehler Avenue - Suite 2
Ronkonkoma, NY 11779) with average thickness 7 nm and 3. Results and discussion
23 Wt.% total graphene content in N-Butyl acetate solvent 3.1 Structural and morphology characterization of
(Zhao et al., 2010; Hummers and Offeman, 1958). The as- graphene nanoplatelets
received GNPs were characterized by SEM (JEOL JSM- Figure 4 shows SEM images (JSM-6010LV; JEOL, Ltd.,
6010LV), Raman spectroscopy (Bruker Sentra) and XRD Tokyo, Japan) of the GNPs at low magnification (a) and high
analysis (XRD-6100; Shimadzu Corporation, Kyoto, Japan) to magnification (b). The drop casted GNPs has an overlapped
ensure its quality. flake structure. In addition, the flakes are superimposed
together and have irregular shapes with a maximum flake size of
2.2 Sensor fabrication 5 m m lateral dimension. Moreover, the flakes are nearly equal
Platinum electrodes were deposited on a thin (100 m m) PET in size, well-dispersed and not arranged in the initial graphitic
substrate using thermal evaporation [Figure 1(a), 1(b)] to form crystalline structure due to the chemical reduction. Most of

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Figure 2 Actual photograph for the fabricated temperature sensor before (a) and after GNPs drop casting (b) Sensor subjecting to bending stress (c)

Figure 3 Test setup for the graphene-based temperature sensor characterization

Figure 4 SEM images of GNPs at different magnifications

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flakes are flat with sharp edges and smooth surface with less Figure 6 XRD spectra of GNPs
pores which reflects the better oxidation and reduction process.
The appearance of wrinkled surface textures with curling edges
is nearly disappeared. Consequently, the agglomeration
process in the GNPs suspension will tend to disappear.
Figure 5 presents the GNPs characterization by Raman
spectroscopy which is the most important technique in
characterizing the structure of graphitic materials (Lab RAM
HR-800; Horiba, Ltd., Kyoto, Japan) (Li et al., 2007). The D,
G and 2D bands of GNPs were appeared at 1346 cm 1,
1577 cm 1 and 2712 cm 1 respectively.
Interestingly, the relative intensity of the D-band (carbon-
carbon sp3 structure), which is related to the GNPs crystal
defects and is known as the disorder band, is very weak. As a
result, the quality of the GNPs is very high and that is considered
as a good indicator of achieving a better GNPs based temperature
sensor. G-band (carbon-carbon sp2 structure) is the main
spectral feature of GNPs, and it is the optical oscillation of carbon
atoms. It indicates to the number of GNPs layers.
2D band is a double resonance stemming from the interaction intensity peak at 2u  27.18° corresponds to a (002) plane with
of two phonons and light. This resonance is associated with the a d-spacing of 3.28 Å refers to the presence of pure GNPs with
electrical structure of the GNPs. Thus, 2D band is extremely the same basal spacing as natural graphite. The low intensity
sensitive to changes in the electronic band structure, which varies peak at 2u  55.24° corresponds to a (004) plane with a d-
depending on the interlayer interactions in the GNPs. The spacing of 1.66 Å confirming that GNPs are not completely
thickness of GNPs decreases when this beak becomes sharper exfoliated, which is in good agreement with the results of
and more symmetrical. Contrary, the thickness of GNPs previous studies (Ferrari, 2007; Li et al., 2011; García et al.,
increases (Few layers) when this peak becomes broader (Ni et al., 2015; Jiang et al., 2018; Stobinski et al., 2014).
2008). From Figure 5, the archived 2D peak is sharp and
symmetric which reflects the low number of graphene layers in 3.2 Sensing characterizations
the GNPs. As a result, high sensor performance is expected. Figure 7 shows the sensor signal (change in resistance) when
Obviously, the intensity of the G band is greater than the 2D the sensor exposed to temperature higher than RT. The cycle
band which refers to multilayer GNPs. In addition, the high IG/ was repeated at various temperatures, where the sensor was
I2D ratio refers to the low number of deposited. Consequently, transferred from RT to the testing chamber which is heated to a
the quality and performance of our fabricated temperature certain temperature and it is hold for 75 sec before it rapidly
sensor are expected to be higher than the fabricated by Sahoo pulled out for cooling to the RT again. The process is repeated
et al. (2012) which has high ID/IG ratio. with increasing the temperature of the heating chamber and the
XRD analyses were carried out to estimate the effectiveness resistance change due to temperature change was monitoring
of the oxidation, expansion and reduction of graphite. Figure 6 with time. The fabricated sensor was subjected to different
shows the XRD spectra of the GNPs (XRD-6100; Shimadzu temperatures start from the RT until 150°C. It is clear that
Corporation, Kyoto, Japan), the presence of a sharp higher the resistance changes (red colour) with the temperature
change (blue colour) and becomes stable once it reaches to the
measured value. Each temperature has its comparable
Figure 5 Raman spectroscopy of the GNPs
resistance. Consequently, the fabricated sensor provides clear
sensing behaviour to the measured temperature. The sensor is
very sensitive to the temperature environment as well as the
whole selected temperature range. The sensor response may be
improved with increasing the temperature with slightly increase
in the response and recovery time constants.
Figure 8 provides the sensor resistance behaviour at
temperature range of RT to 150°C. The resistance changes
linearly with the temperature change according to the linear
equation R = 60.17 1 0.0845 t (oC), obtained from line fitting for
the measured data. The resistance changes directly proportional
with the temperature which confirms the results obtained by
Benyamin Davaji et al. (2017). An ideal temperature sensor
would have a perfectly linear response: a unit change in
temperature would result in a unit change in resistance output
across the entire temperature range of the sensor. However, no
sensor is perfectly linear. The non-linearity of our fabricated
sensor was approximately 0.36%, where the non-linearity was

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Figure 7 Effect of temperature (60°C – 150°C) on resistance change at time intervals

Figure 8 Resistance change with temperatures change increase (Dewapriya et al., 2013). Secondly, The phonon and the
electron coupling rate in the GNPs film increases, which
decreases the quasiparticle weight of the electron excitation and
affects the electron movement in the GNPs (Tian et al., 2014).
The TCR which explains the rate of change of the sensor
resistance per 1°C (a) is calculated from the equation a = (1/Ro)
(dR/dT). Where, Ro is the initial resistance of the sample at RT
and dR/dT is the slope. The calculated value of the TCR for our
fabricated sensor is 1.4  10 3/°C which is in consistence with
the obtained value by Satyaprakash Sahoo et al. (1.95  10 3/°C)
for reduced graphene oxide (RGO) (Sahoo et al., 2012) and
twice the measured for carbon nanotube (CNT) film
(0.7  10 3/°C) (Di Bartolomeo et al., 2009). Interestingly, it is
also very close to the measured for single layer graphene resistor
( 1.47  10 3/°C) (Cheianov and Fal’ko, 2006) and for CNT
(1.3  10 3/°C) (Husain and Kennon, 2013). Moreover, it is
three times nearly if it is compared with graphite (0.5  10 3) (Ali
and Hafez, 2013) as tabulated in Table 1.
Figure 9(a) presents the effect of repeatable heating and
cooling on our fabricated temperature sensor (blue). To ensure
the repeatability and stability of our sensor, we have heated the
sensor to 150°C, holding for approximately 75 sec and then
cooling to the RT. The heating-cooling process was repeated
calculated by dividing the maximum output error from the linear several times to ensure its repeatability and stability. It was found
fit at 130°C by the actual measured value (70.9 X) at same that the fabricated sensor provides repeatable measurements with
temperature. Consequently, our fabricated temperature sensor is stable values through the holding time (75 sec). In parallel,
strongly recommended to be commercialized due to its very low Figure 9(b) provides the measured furnace temperature (red)
non-linearity. with time by a commercial temperature sensor. It is clear that the
The sensor resistance depends on the conduction electrons. By furnace temperature is nearly stable with time and that
increasing the furnace temperature, the number of electrons will strengthen our measured values, where the very small fluctuation
be increased and causes scattering increase. As a result, the in the furnace temperature is also appear in our sensor resistance.
mobility of the electrons will be decreased and the resistance
increases with temperature increase (Xi et al., 2014; Yin et al.,
2014; Akturk and Goldsman, 2008). The mobility depends not
only on temperature but also on various scattering mechanisms, Table 1 TCR values for deferent materials used for temperature sensing
such as defects, phonons, surfaces and edges (Zhu et al., 2009; Sensor material TCR/°C Ref.
Hwang et al., 2007; Sun et al., 2013). In More details, we can –3
GNPs 1.4  10 This work
divide the effect of temperature on the resistance change of GNPs
RGO 1.95  10–3 Sahoo et al. (2012)
into two basic factors. Firstly, the stacked layers of graphene
CNT film 0.7  10–3 Di Bartolomeo et al.
within the GNPs flakes have good conductivity at RT but with
(2009)
increasing the temperature the trapped air between graphene
Single layer graphene resistor 1.47  10–3 Cheianov and Fal’ko
layers or inside the pores will expanded and the wrinkled surface (2006)
will increase due to thermal disturbance. As a result, the contact CNT 1.3  10–3 Husain and Kennon
areas between the graphene sheets will be decreased and the (2013)
distance between the graphene layers will increase. Graphite 0.5  10–3 Ali and Hafez (2013)
Consequently, the resistance will increase with the temperature

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Figure 9 Sensing repeatability at 150°C overlapped flake structure and each flake has a multi-layer of
the graphene sheets staked together. Ideally, these flakes are
homogeneous and in perfect contact with each other’s. In fact,
the flakes are irregular and have defects, pores and wrinkled
surface textures with curling edges as illustrated by SEM and
Raman spectroscopy shown in Figures 4 and 5. With the
temperature increase the defects, pores and wrinkled surface
textures may increase or decrees based on the temperature
coefficient of expansion. The air filled the pores has a great
effect on the heat-transfer resistance. As a result, it will cause a
significant effect on the response time. In general, Increasing
the temperature can cause an increase or a decrease in response
time depending on how temperature affects the material
properties and heat transfer inside the sensor. As such, the
effect of temperature on sensor response time can only be
identified by in-situ testing of response time at process
operating temperature (Hashemian, 2006). Thus, we tested
our fabricated sensor at different temperatures for response
time investigation.
The observation confirmed the high sensitivity of the sensor for Figure 11 represents the response time (red), recovery time
the change in the temperature. (green), polynomial fit of response time (black) and polynomial
Figure 10 represents the sensor stability at two different fit of recovery time (blue) of our fabricated temperature sensor.
applied temperatures (40°C and 100°C). To study the stability The response time was measured by heating the fabricated
of our fabricated sensor, we subjected it to a fixed temperature sensor from RT up to the pre-ascribed temperature. Contrary,
for 6 hours and we recorded the measured temperature every the recovery time was measured by cooling the sensor from the
30 min. It was found that our fabricated sensor provides a good measured temperature to the RT. The response and recovery
times were measured for a temperature range from 60°C to
stability with a fluctuation range less than 1 X. The present
150°C with 10°C step increase. The response and recovery
fabricated sensor provides more stability than the fabricated
times are considered as 90% from the measured steady state
one by Tian et al. (2014).
temperature. The response times are much faster than the
The response time of the resistance-based temperature
recovery times. Moreover, the response and recovery times
sensor is affected by the temperature change because the
increase with increasing the measured temperature. For
change in temperature has a direct effect on the heat transfer
instance, at 60°C the response and recovery times were 3.0 and
between the sensor and the surrounding environment (Air).
7.0 s, respectively. Meanwhile, at 150°C the response and
Moreover, it has a great effect on the sensor dimensional
recovery times were 9.5 and 15.5 s, respectively. Interestingly,
change (Hashemian, 2006; Zeng et al., 2019).
the curves of response and recovery times were found to be well
The sensor dimensional change due to temperature change is
fitted with the second-degree polynomial equations tRes =
the most dominant factor on the response time. The fabricated
5.55682 1 0.17064 T- 4.73485  10 4 T2 and tRec =
GNPs resistance-based temperature sensor consists of

Figure 11 Sensor time response and recovery


Figure 10 GNPs temperature sensor long hour stability at
temperatures 60°C and 100°C

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5.23409 1 0.23799 T - 6.62879  10 4 T2, respectively. Figure 13 Effect of relative humidity on the relative resistance of the
Where, tRes, tRec and T are the response, recovery times in fabricated temperature sensor
seconds and T is the measured temperature in degree Celsius,
respectively. The obtained results for recovery time are in a
consistent trend with the measured for GNWs by Yang et al.
(2015). However, the response time is decreased with
temperature increase. Table 2 provides a clear comparison
between our fabricated sensor and other GNPs and graphene
derivatives. Interestingly, our fabricated temperature sensor
provides a better response and recovery times.
One of the interesting curves is the calibration curve of the
fabricated sensor, shown in Figure 12. The sensor response
is defined here as the resistance of the sensor at the
measured temperature divided by the resistance at RT (S =
Rt/R(RT)). The sensor response shows a linear behaviour,
where a soft increase in the sensor response is observed with
increasing the temperature. The sensor responds to the low
and high temperature, which gives the present sensor an
advantage. The sensor response is well fitted with the
straight-line formula of S = 0.95231 1 0.00134 t (oC). Form
this equation we can determine the temperature of the
ambient or medium atmosphere with the measuring the
sensor response. The effect of humidity on the performance of our fabricated
temperature sensor is applied by subjecting it to different
humidity levels using a controlled humidity chamber
(Humidity Series, Sheldon Manufacturing, Inc.). Figure 13
Table 2 Response and recovery times for different temperature sensors
presents the effect of relative humidity change on the relative
Temperature Response Recovery resistance of our fabricated sensor. The sensor resistance upon
Sensor material (oC) time (S) time (S) Ref. exposure to the humidity did not change until 50% humidity,
GNPs 100 7 12 This work however, slightly increased with higher humidity. It was found
40 0.5 3.2 that the maximum relative resistance change at 80% humidity
PEDOT:PSS- 100 18 32 Soni et al. is less than 0.05 which can be neglected compared to the
Graphene Oxide (2020) change in relative resistance (sensor response) with the change
Commercial 65 120 in the temperature. The results confirm that the present sensor
thermistor (100 KX) has a capability to work at various levels of humidity conditions
GNPs 40 7 60 Tian et al. with neglected effect of humidity.
MWCNTs 17.1 60 (2014)

4. Conclusions
In summary, we present the fabrication of an efficient and
Figure 12 The calibration curve of the sensor response as a function of
reliable GNPs resistive-based temperature sensor on a PET
the temperature
substrate by simple, easy and low-cost technique which can be
readily used in practice. Based on the mentioned results we can
conclude the followings:
 The fabricated sensor showed a good response toward the
different temperatures (RT to 150 °C) and its
corresponding resistance was measured.
 A linear relationship between the temperature and
the resistance was achieved, which allow us to calculate
the temperature coefficient of resistance (TCR) of the
fabricated sensor to be found as 1.4  10 3/°C.
 The sensor also showed excellent repeatability and
stability for the measured temperature range, with
acceptable response and recovery times.
 Excellent sensor response showed a good linearity with
temperature change, thus, with known the sensor
response, the ambient temperature can be determined
based on the calibration curve.

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Tian, M., Huang, Y., Wang, W., Li, R., Liu, P., Liu, C. and Corresponding author
Zhang, Y. (2014), “Temperature-dependent electrical Mohammed Gamil can be contacted at: mohammed.
properties of graphene nanoplatelets film dropped on flexible gamil@feng.bu.edu.eg

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