Graphene Based Smart Sensors

Sensors and Actuators A 270 (2018) 177–194
Contents lists available at ScienceDirect
Sensors and Actuators A: Physical

journal homepage: www.elsevier.com/locate/sna
Review
Graphene and its sensor-based applications: A review

Anindya Nag a,∗ , Arkadeep Mitra b , Subhas Chandra Mukhopadhyay a
a
Faculty of Science and Engineering Macquarie University, Australia
b
Department of Electrical Engineering University of Texas, Arlington, USA
a r t i c l e i n f o a b s t r a c t
Article history: This paper presents an overview of the work done on graphene in recent years. It explains the preparation
Received 7 September 2017 techniques, the properties of graphene related to its physio-chemical structure and some key applications.
Received in revised form Graphene, due to its outstanding electrical, mechanical and thermal properties, has been one of the most
28 November 2017
popular choices to develop the electrodes of a sensor. It has been used in different forms including
Accepted 12 December 2017
nanoparticle and oxide forms. Along with the preparation and properties of graphene, the categorization
Available online 29 December 2017
of the applications has been done based on the type of sensors. Comparisons between different research
studies for each type have been made to highlight their performances. The challenges faced by the current
Keywords:
Graphene
graphene-based sensors along with some of the probable solutions and their future opportunities are also
Electrochemical sensors briefly explained in this paper.
Strain sensors © 2017 Elsevier B.V. All rights reserved.
Electrical sensors
Nanocomposite
Contents
1. Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 177
2. Preparation of graphene . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 179
2.1. Chemical vapor deposition . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 179
2.2. Mechanical exfoliation . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 180
2.3. Hummer’s method . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 180
3. Properties of graphene . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 180
4. Electrochemical sensors . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 183
5. Strain sensors . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 184
6. Electrical sensors . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 186
7. Challenges with the current sensors . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 186
8. Conclusion . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 187
9. Future opportunities . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 188
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 190
Biography . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 194
1. Introduction allow the monitoring unit to receive and analyze the sensed data.
Research work has been going on continuously to develop the mate-
After the advent of smart sensors around two decades back [1], rials used for electrodes. Existing materials have been improved
their applications in daily life have been ever increasing. Nowadays, based on their mechanical, electrical and thermal properties. Gold,
almost every industrial, domestic and environmental sector utilizes silver, aluminum and carbon are some of the commonly used mate-
sensors for improving the quality of life [2–7]. Among the senso- rials used to develop electrodes [8–10]. Out of them, graphene
rial parts, electrodes constitute the most important section as they has always been a popular choice due to its distinct advantage of
exhibiting excellent electrical and crystal qualities. Graphene, in
simple words, can be defined as a single layer of carbon atoms that
∗ Corresponding author. are tightly packed to form a 2D honeycomb crystal lattice structure
E-mail address: anindya.nag@students.mq.edu.au (A. Nag). [11].
https://doi.org/10.1016/j.sna.2017.12.028
0924-4247/© 2017 Elsevier B.V. All rights reserved.
178 A. Nag et al. / Sensors and Actuators A 270 (2018) 177–194
Fig. 1. Different forms (0D, 1D and 3D) of modified graphene [11].
It is the basic component for the carbon allotropes which can bination of all these aspects is yet to be done. The motivation of
be modified into other forms like 0D fullerenes, 1D CNTs, and 3D this review article is to present a general overview of the impor-
graphite as shown in Fig. 1. The work on graphene has been going tance of graphene as a material, its preparation, and utilization in
on for the last sixty years, but earlier, it was mostly described as an some of the significant aspects. It showcases the different prop-
allotrope of carbon to explain different carbon-based materials. It erties of graphene which makes it a superior element that can be
was just in recent times, around a decade back, the free-standing considered for dynamic applications. It also shows a comparative
2D model of graphene was experimentally proved [12,13]. In the study in the form of tables to highlight the performance of different
applied field of research, among its wide range of applications, research studies done on graphene-based electrochemical, strain
graphene has been mostly used in batteries and cells as anodes, and electrical sensors. The paper also depicts the strength and lim-
and in supercapacitors due to its low charging time, high strength itations of the current sensors along with the challenges and future
to weight ratio, and large surface area. It has also found a large opportunities of graphene-based sensors.
number of applications in areas like sensors, biomedical engineer- The involvement of graphene to develop sensors is attributed to
ing, nano and flexible electronics and catalysis due to its unique some of the distinct advantages like the large surface-to-volume
properties which include a distinctive nanopore structure, high ratio, unique optical properties, excellent carrier mobility and
mechanical strength and high electrical and thermal conductiv- exceptional electrical and thermal properties compared to the
ity. The functionalization of graphene, to reduce the cohesive force other allotropes of carbon. These properties are constant for the
between the graphene molecules in different forms, has caused sig- double and multi-layered graphene structures. Apart from the
nificant changes in its physicochemical properties, thus increasing difference in the structure, working conditions, the use of these
their end applications [14–20]. Two different forms of function- advantages in graphene sensors lie mainly in their capability to
alization, covalent and non-covalent, are achieved for graphene adjust according to the application. For example, in strain sensors,
molecules when the materials are chemically treated by different properties like the detection limit, maximum sensing range, sig-
techniques like spin-coating, filtration, layer-by-layer assembly to nal response and reproducibility of the response hold a pivotal role
cause surface modification but maintaining its intrinsic properties to determine the quality of the sensor. These characteristics are
[21]. Even though a lot of research articles have been published attributed to the electrical and mechanical properties of graphene.
based on the different techniques for the preparation of graphene In electrochemical sensors, its large surface area helps the loading
and its utilization in sensors, a thorough research work on the com- of the desired biomolecules, resulting in the interaction between
A. Nag et al. / Sensors and Actuators A 270 (2018) 177–194 179
Table 1
Comparison between the different characteristics of strain sensors where the electrodes are developed with graphene, CNTs and silver.
Electrode material Gauge Factor Maximum attainable strain (%) Linearity in the response Reference
Graphene ∼106 120 Non-linear up to 1% [24]

103 106.2 Linear up to 6% [25]
29 70 Linear up to77% [26]
300 <30 (Tunable GF) Linear [27]
15-29 70 Linear [26]
7.1 100 Linear [28]
Carbon Nanotubes 12.1 410 Linear [29]

(CNTs) 0.82 280 Two linear regions [30]
8.7-62.3 100 Non-linear [31]
0.99 100 Linear [32]
1 150 Linear [33]
0.97 300 Linear [34]
Silver 2-14 70 Linear up to 40% [35]

0.7 50 Linear [36]
1.07-12.4 100 Non-linear [37]
1 50 Linear up to 80% [38]
1 170 Linear up to 60% [39]
24-95 102 Linear [40]
Table 2
: Comparison between the different characteristics of the electrochemical sensors where the electrodes were developed with graphene, CNTs and silver.
Electrode material Limit of Detection Sensitivity Linear range References

−1 −2
Graphene 0.2 ␮M 31.2 ␮A mM cm 1.0 ␮M– 1.0 mM [41]
6.9 ␮M 266.6 ␮A mM−1 cm−2 3.5 mM [42]
0.2 ␮M 31.2 ␮A mM−1 cm−2 1.0 ␮M–1.0 mM [43]
0.015 ␮M 0.204 ␮A/␮M 0.05–780 ␮M [44]
1.73 ␮M 0.085 ␮A ␮M−1 cm−2 0.5–3 mM [45]
6.9 ␮M 266.6 ␮A mM−1 cm−2 0– 3.5 mM [46]
Carbon Nanotubes 2.1 × 10−7 M 7.0 × 10−7 –3.5 × 10−3 M 17.76 ␮A mM−1 [47]
(CNTs) 10 ± 2 ␮M 0.1–10 mM 10 ± 3 ␮A mM−1 cm−2 [48]
1.29 mM 6800 nA mM−1 1.29–12.93 mM [49]
4.0 × 10−6 M 0.54 ␮A mM−1 8.0 × 10−6 –4.5 × 10−4 M [50]
0.2 ␮M 2596 ␮A mM−1 cm−2 0–1.2 mM [51]
Silver 29.2 ␮M 0.0266 ␮A cm−2 ␮M−1 0.1–3.1 mM [52]

49 nmol dm–3 0.49 ␮A/␮mol dm–3 0.40 ␮mol dm–3 –2.0 mmol dm–3 [53]
1 × 10−7 M 1043 ␮A mM−1 cm−2 5.0 × 10−7 –7.0 × 10−3 M [54]
2.83 ␮M 0.4 ␮A/V 10 ␮M –0.8 mM [55]
1.2 nM 2.55 ␮A ␮M−1 4.8 nM–0.31 ␮M [56]
0.2 ␮M 57.5 ␮A mM−1 cm−2 0.2 Mm–70 mM [57]
the analyte molecule and electrode surface due to the high bal- 2.1. Chemical vapor deposition
listic transport capability and the very small band gap. Another
advantage of graphene lies in its low environmental impact, mak- In an environment of an inert gas like N2 a quartz-tube furnace
ing it more popular for sensing purposes than other metals [22,23]. [58] is heated and on peaking the deposition temperature carbona-
Tables 1 and 2 show the comparison of the performance of some of ceous gases of mixture of Ar/H2 /CH4 [59–61] the passed through
the electrochemical and strain sensors developed with graphene varying dimensions such as one sq. inch Ni/Cu/Co/Pt/Ir/Nu metal
with that of Carbon Nanotubes (CNTs) and silver. It is seen from that is placed in the furnace. The gases deposit carbon in the metal
Table 1 that the Gauge Factors (G.F.) and maximum attainable at elevated temperature, forming a single long atom-thick mono-
strain are mostly highest for the graphene-based sensors. One dis- layer/multilayer of graphene over a prolonged period. To control
advantage of these sensors is the variation in the linearity in their and reduce manufacturing process temperature, plasma without
response. For the other two types of sensors, the GFs are much less a catalyst is used in the chemical vapor deposition (CVD) process
than graphene sensors, even though most of them attain a fairly [62,63]. Graphene CVD synthesis utilizing waste products is done
high amount of detectable strain. It is seen from Table 2 that, even by placing sustainable materials like butter, camphor (C10 H16 O)
though the limit of detection achieved by all the three different (with/without iodine), tea tree (Melaleuca alternifoliate) extrac-
types of sensors is the same, most of the graphene based sensors tion, waste plastic (solid form), cookies, chocolates over Ni foam,
are able to achieve high sensitivity with a wider linear range. Ni/Cu metal foils, polycrystalline Ni in an atmosphere of Ar+H2 ,
H2 , Ar at normal /ambient pressure, elevated temperature and RF
2. Preparation of graphene power for a period of time. A summary of some of the selected con-
ditions for the preperation of graphene using CVD along with other
Optimization of the preparation of graphene has been per- methods are given in Table 3.
formed for some years, since its invention and application. Some
of the significant methods that are used worldwide to generate
graphene on a large scale are given below.
Table 3
: Summary of some of the selected conditions of preparation of graphene using different methods.
Technique Gas source/reducing agent Temperature (◦ C) Substrate References
SWP-CVD CH4 :Ar:H2 300 − 400 Cu, Al [75]

MWCVD MWCVD 450 − 750 Ni [76]
LPCVD CH4 1000 Cu [77]
APCVD CH4 :H2 :Ar 960–970 Ni [78]
LPCVD CH4 :H2 :Ar 900 Ni,Cu on SiO2 /Si [79]
Mechanical exfoliation – 25 SiC [80]
Mechanical exfoliation – 25 Si [81]
Mechanical exfoliation – 25 HOPG crystal [82]
Mechanical exfoliation – 1000 NaCl crystallites [83]
Hummer’s Method KMnO4 , H2 SO4 20 – [68]
Hummer’s Method KMnO4 , H2 SO4, H2 SO4 and H3 PO4 25 – [72]
Hummer’s Method NaNO3 , H2 SO4 0 – [84]
Hummer’s Method NaNO3 , KMnO4, H2 SO4 150 – [85]
2.2. Mechanical exfoliation by studying the XRD, FTIR, SEM, TEM and Raman spectra. Mul-
tiple graphene layers are obtained, when, before being subjected
Scotch tape is used primarily, in this method to stick over the to chemical cleaning and ultrasound treatment, in an N2 environ-
graphite crystals or graphite flakes [64]. The tape leads to the ment at a feverish temperature, dead camphor leaves are subjected
entrapment of graphite layers. The tape is repeatedly peeled and to pyrolysis. Graphene is yielded when coal-tar pitch (CTP) is sub-
observed under the microscope over a prolonged period to extract jected to spin coating on Si, followed by annealing with a Ni layer at
the graphene layer. The experiment can be repeated with a silicon elevated temperature, low vacuum and normal atmospheric con-
wafer that is oxidized [65]. This method is considered analogous ditions [73,74].
to rubbing of a graphite pencil in between two terminals of lead
attached to the package, such that the lead grows once the graphene
sheet has been extracted [66]. However, this method is not favor- 3. Properties of graphene
able for the mass-scale production required for industry [67].
Semi-metallic graphene consists of an arrangement of hexag-
onal covalently bonded one-atom-thick [86,87] carbon atoms
2.3. Hummer’s method arranged together in a honeycomb lattice structure. Out of four
carbon atoms, three carbon atoms exhibit sp2 hybridization. By
Graphite powder is one of the most important constituents the hybridization, the trigonal system of carbon atoms exhibits a
of the low-cost Hummer’s process [68]. Over the past few years, high bonding energy (∼5.9 eV), separated with sigma bonds with a
methods have been devised to obtain graphite powder from waste bond length of 1.42 Å. The lone p-orbital, being half filled, forms
products [69]. One such procedure involves utilization of zinc- pi bonds with the adjacent carbon atoms [88,89]. The slippery
carbon batteries [70]. Electrodes from the waste batteries are graphene sheets are normally one atom thick and are stacked one
grounded into graphite powder after being subjected to washing above another to form the graphite 3D structure. The sheets are held
for removal of impurities, before being treated with a solution of together by the weak Van der Waal’s forces. The slippery nature of
HCl: HNO3 in the ratio of 3:1. The total solution is further subjected the sheets can be attributed to the presence of vibrational phonons,
to extreme heating, centrifuge, water treatment followed by drying which also happen to be present in the 3D solids. Figs. 2 and 3
at a fairly high temperature for a prolonged period, finally obtaining depict the schematic diagram of the honeycomb lattice structure
purified Graphite powder. In another procedure, bagasse or waste of graphene and its electron dispersion phenomenon in a defined
sugar cane, when finely ground, mixed with ferrocene and passed energy spectrum respectively.
through a furnace in a crucible for 10 min yields graphite powder.
The modified Hummer’s method eliminates the usage of NaNO3 . a √ a √
a1 = 3, 3 , a2 = 3, − 3 ,
The method involves mixing of H2 SO4 and H3 PO4 at a ratio of 9:1 2 2
[71,72]. Upon mixing the solution is stirred. During stirring graphite
2
√ 2
√
powder and KMnO4 are added slowly. To reduce the temperature The reciprocal vectors are:b2 = 3a
1, − 3 , b1 = 3a
(1, 3)
of the suspension KMnO4 is added slowly. Continuously stirring is
done for 6 h such that the color changes to dark green. A small quan- a √ a √ 2 √ 2 √
a1 = 3, 3 , a2 = 3, − 3 , b2 = 1, − 3 , b1 = (1, 3)
2 2 3a 3a
tity of H2 O2 is added to halt the copious production of KMnO4 . The
H2 O2 containing total mixture is stirred for a brief time. The excess
heat producing reaction is left for cooling in an ice bath. HCl and DI
The magnitudes
of the corners
of the Brillouin zone of graphene
2 2 2 2
water are further added to the solution for removal of metal ions. are: K = , √
3a 3 3a
,K = 3a
, − √
3 3a
The solution is subjected to centrifuge systems at high speed for a
short duration. The particles left over are washed with hydrochloric a √ a √
∂1 = 1, 3 , ∂2 = 1, − 3 , ∂3 = −a(1, 0)
acid and de-ionized water thrice before being subjected to intense 2 2
heat in the oven for a prolonged period to produce Graphene oxide

(GO) in powdered form. The Graphene Oxide is further mixed with K= 2
, √2
, K = ( 2 ,− 2
√ ) Magnitude of the vectors
3a 3 3a 3a
water and was subjected to ultrasonication for a stipulated amount a
√ a
√
3 3a
of time. Sulfur-laced reducing agent (NaHSO3 , Na2 S.9H2 0, SO2 ) in a are:∂1 = 2

1, 3 , ∂2 = 2
1, − 3 , ∂3 = −a(1, 0)
very small amount is added to the mixture at an elevated tempera- Nearest neighbors are located at∂1 = ±a1 , ∂2 = ±a2 , ∂3 =
ture and low, stirring speeds for a long time. The mixture is further ±(a2 − a1 )
subjected to filtration and DI water washing multiple times. Upon
freeze drying, powdery black graphene is obtained. The quality of ∂1 = ±a1 , ∂2 = ±a2 , ∂3 = ±(a2 − a1 )
graphite oxide, graphene oxide and graphene can be determined
Fig. 2. Schematic diagram of the structure of graphene represented in the form of a Honeycomb lattice and its Brillouin zone [90].
Fig. 3. Electronic dispersion of the honeycomb lattice in terms of (zoomed in) the energy spectrum of finite values [89,90].

The Hamiltonian has magnitude:H = −t a+ b + H.c. −
,i ,j The massless Dirac fermions are the unique characteristics of
i,j, graphene. The Dirac fermions travel at a speed (≈106 m/s) less than

that of light. The Dirac fermions are not affected by external electro-
t (a+ +
,i a,j + b,i b,j + H.c.) static potentials exhibiting Klein Paradox, and lead to the integer
i,j, quantum hall effect, by which the chance of electrons crossing a

potential barrier is always unity [90–92]. The incident Dirac elec-
H = −t a+ b + H.c. − t
,i ,j
(a+ +
,i a,j + b,i b,j + H.c.) trons don’t get reflected and propagate with 100% efficiency in cases
i,j, i,j, where the internal scattering and symmetrical aspects of carbon
atoms are neglected. The chances of reflection at angles greater
Energy bands have the magnitude:E± (k) = ±t 3 + f (k) − than zero degrees depend on more of the barrier changing at a

t f (k) slower pace. The Dirac fermions are however affected by localized
√ electrons, leading to the jittery characteristics. An inverse relation-
√ 3 3 ship between electrons and holes is exhibited between velocity and
f (k) = 2cos 3ky a + 4cos ky a cos( kx a)
2 2 momentum. The photons, like electrons, always try to search for a

hole to form an image on the screen. The quasiparticles overlap
E± (k) = ±t 3 + f (k) − t f (k)where f(k) is represented by: with the Quasi-holes of another band on the condition that the
√ √
distance between the Dirac and Fermi energies are less than the
f (k) = 2cos 3ky a + 4cos 23 ky a cos( 32 kx a)
superconducting distances.

Graphene’s high electrical conductivity (∼1.0*108 S/m),
4
E
1 Z1 high melting point (4510 K), high thermal conductivity
(E) = 2 2 F ,
(2000–4000 W m−1 K−1 , 5000 W/m K), highest current den-
t Z0 2 Z0
sity (∼1.6*109 A/cm2 ), including a high electron mobility

(200,000 cm2 V− 1 s−1 at electron density ∼2*1011 cm-2 ) con-
2Ac
E
tributes to its application in electrochemical sensors, strain
(E) = sensors and electrical sensors that are discussed in detail in a later
v2
F
section of the paper [93–95]. The chirality of graphene is exhibited
by straight, armchair and zigzag geometry. The zigzag geometry
4 |E | √1 F( 2 , Z1
(E) = Z0
)The values of Z1 and Z0 vary is more in control of states and resonances. The magnitude of the
2 t 2 Z0
for different intervals. The DOS near the Dirac point has the tensile strength, shear modulus, and Poisson’s ratio varies for each
c |E | of the chiral geometries, and are summarized in Table 4 [96].
magnitude: (E) = 2A 2 vF
Table 4
Comparison between the geometrical patterns of the single-layered graphene sheets [96].
Geometry a (nm) b (nm) Young’s modulus (TPa) Shear Modulus (TPa) Poisson’s Ratio
Zigzag 6.395 4.184 1.040 0.213 1.441

Armchair 6.153 4.263 1.042 0.228 1.285
Chiral 4.713 3.256 0.992 0.233 1.129
Steel’s tensile strength is less [97] than for graphene (∼130 GPa) Some of the popular applications like electrochemical, strain
[93], which may be used in structural engineering applications like and electrical sensing with graphene based sensors have been
that of aeroplane [98] composites. Graphene’s elastic property is addressed in the succeeding sections. There are distinct advantages
such that a 20% increase along its length doesn’t compromise its of graphene for which it is chosen for these specific applications.
properties [99]. It’s very high surface area (∼2600 m2 /gm) can con- It exhibits less electrical noise and crystal defects than conven-
tribute to its application in fire-fighting appliances [100]. tional sensing materials. Moreover, the electrochemical sensors
The characterization of graphene is done using various tech- developed with graphene can be operated with simpler techniques
niques like X-ray diffraction (XRD), Fourier transform infrared than conventional methods like that of the mass spectrometer
spectrum (FTIR), Ultraviolet–visible (UV–vis) spectroscopy, Scan- [106]. Other advantages would be its robustness, high flexibility,
ning Electron Microscopy (SEM) and Transmission Electron and electrical conductivity. These are the attributes for which it
Microscopy (TEM) and X-ray photoelectron spectroscopy (XPS). is used for developing electrochemical sensors for the detection
The XRD is done to investigate the phase and structure of the fab- of hazardous substances like hydrazine and selective detection of
rication samples. In one of the research [101], the diffraction peak hemoglobin, adenine dinucleotide and biomolecules like ascorbic
obtained at 2␪ = 10.2◦ for the graphene-CdS nanocomposites, corre- acid, uric acid [107–111], etc. In these applications, nanocomposites
sponds to the (0 0 1) reflection of graphite oxide. The peaks obtained have been formed by mixing pure graphene with other materials
with the samples are correlated to the structure of the compound like Platinum (Pt), TiO2 to increase the sensitivity and detection
under consideration. The alignments of graphene grown on dif- capability of the sensor. When any gas is brought through channels
ferent substrates are studied with XRD determining the crystal in low concentrations, then made to flow through the graphene
directions. The diffraction peaks and d- spacing obtained for the surface, this causes an immediate effect on its charge concentra-
nanocomposites are generally higher than those of the pure mate- tion. The difference in charge concentration brings a corresponding
rial. This is due to the random positioning of the filler inside the change in the resistance, conductivity values of graphene [112]. The
polymer matrix. The peak and spacing values gives a very good indi- values help in interpreting the nature of the gas molecules. The
cation of the degree of dispersion of the fillers in the matrix. The graphene-based chemical sensors can be manufactured cheaply
SEM and TEM images are also studied by placing a section of the using acrylic plastic as a substrate. Avoiding e-beam lithogra-
material in an illuminated area at different orientations to deter- phy and other sophisticated techniques of lithography also, brings
mine the features of developed sensors in the nanometer domain. down the manufacturing cost and time. Moreover, the switching
Different types of TEM like High-Resolution TEM (HRTEM), Dark- time for a graphene based electrochemical sensor involving a dual
Field TEM (DFTEM) are studied depending on the resolution of the channel of inlet gas and analyte gas, the switching times in between
fillers in the material. The top and cross-sectional views of the SEM the two gases is very small. The less weighty graphene chemical
images are another parameter for analyzing the dispersion of the sensor is wearable, operates at normal atmospheric pressure and
fillers [102]. The FTIR studied for the graphene-based nanocom- room temperature. The unique relationship between the mechan-
posites determines different ranges of wave numbers with respect ical and electronic properties of graphene has also helped it to
to transmittance to analyze the elements present in the nanocom- be used for strain sensing. Due to a high mechanical stiffness of
posite. The stretching and deformation vibrations of the functional around 1 TPa and an intrinsic breaking strength of 130 GPa, they are
groups are mainly studied with this technique. The absorption considered to be the most robust and powerful material. This has
bands related to the transmittance vary according the functional been combined with some of the electronic properties like the high
groups present in the nanocomposite. The peaks of the different velocity of electrons (1/100 velocity of light) and a zero band gap
bands in the FTIR are also studied to determine the vibrations of to form graphene-based strain sensors. Mostly for strain sensing,
the adsorbed molecules on the graphene domains. A comparative graphene in different forms like rGO has been mixed with poly-
study between the developed nanocomposite and pure graphene mers like PDMS to achieve highly elastic sensors. Some of them
is generally done to study the C O stretching vibrations, C O H would have gauge factors as high as 630 formed by the selective
deformation vibrations and C O stretching of COOH groups. The coating process. The carrier mobility and electron transfer rate of
contents of the raw materials are varied based on the wave num- graphene at ambient temperature are also very high due to its
bers to optimize the properties of the resultant sensors. UV–vis large surface-to-volume ratio [113–116]. Its unique structure has
spectroscopy, similar to the FTIR, is studied in terms of absorption also caused certain phenomena like the Hall Effect, Klein tunnel-
spectra with respect to wavelength to analyze the peaks corre- ing to take place. Due to these characteristics of graphene, a lot
sponding to the graphene present in the compound. Different of research work has been going on for the last decade, especially
ranges of absorption spectrum are studied in UV–vis spectroscopy in the areas of photonics and optoelectronics. Optical modulators
with a spectrophotometer to study the ␲- bonding between the with a modulating capability of frequencies over 1 GHz of guided
carbon atoms. The absorption peaks may differ from each other, light have been developed by tuning the Fermi levels of graphene
depending on the degree of coupling taking place between the indi- sheets. The high carrier saturation velocity and insensitivity of its
vidual elements in the compound. XPS is another technique, similar response towards temperature variations have led it to find var-
to UV–vis spectroscopy, which is used to study the surface com- ied applications in infrared imaging and optical communications.
positions of the samples. The peaks obtained in XPS are studied Graphene has also been enlisted to develop ultrafast fiber lasers
to analyze the binding energy between the graphene and the sub- by integrating it into different configurations and without affect-
strate. The binding energies in XPS are also attributed to the carbon, ing its alignment [117–120]. An output power gain of 1.55 ␮m has
oxygen and hydrogen bonding with other carbon atoms [103–105]. been achieved with these lasers operating at a wavelength of 2 ␮m.
Fig. 4(a)–(c) show the sensing mechanisms for the three different
Fig. 5. Different protein molecules being wired by graphene on the glassy carbon
electrode [131].
surface for direct electron transfer (DET) reactions. One of the ways
Fig. 4. Schematic diagram of the sensing mechanisms of graphene-based (a) elec- of combing an enzyme on the electrode surface with graphene is
trochemical (b) strain (c) electrical sensors.
via a wiring technique as shown in Fig. 5 [130,131].
Different kinds of enzymatic reactions have been performed
applications using graphene based sensors. It exhibits magnificent where graphene has been conjugated with materials like Chitosan,
electrochemical properties like a large potential window and a low gold (AuNP) and platinum nanoparticles (PtNP), Iron oxides, and
charge-transfer resistance. The electrochemical activity of different PVDF to form nanocomposites on the electrode surface of glucose,
biomolecules using graphene is assisted by its high charge-carrying cholesterol, and hemoglobin sensors [132–138]. Graphene in its
capability and super electrical conductance [121]. In the case of pure, oxide and bio-composite forms has been modified with dif-
strain sensing, the use of graphene as electrodes is highly favorable ferent nanoparticles, nanocubes and nanofibers to develop glucose
due to their highest in-plane electrical conductivity and Young’s sensors [139–144].
Modulus (around 1 TPa for ideal graphene) which gives it high elas- Cholesterol sensors mainly involve the formation of biocom-
tic stiffness and strength. The structural strength and load transfer posites with different polymers. Another form of electrochemical
capabilities of graphene allow it to be intertwined with other con- sensing involves immuno-sensing, where graphene has been used
ductive materials like CNTs and polymers like PDMS, PMMA to as both a label bearer and a non-label bearer element for the detec-
improve the latter’s ability to withstand large cyclic strains of over tion of antigen-antibody recognition sites. When graphene was
50% without having an effect on the sensitivity, response, and used as a label bearer, it was conjugated to antibodies and other
durability. Due to its excellent conductive and elastic properties, particles to develop large electroactive molecules [145–148].
researchers have tried to develop buckling effects of graphene with As a non-label bearer, the conductive material was used on
different forms like ribbons and nano-sheets [122–127]. Some of the surface of the electrode to detect the labels. DNA sensors are
the attributes which caused the use of graphene in electrical sensors another form of electrochemical sensing where the DNA sequences
are its low resistivity, environmental stability, low signal-to-noise or the mutated genes were detected with graphene associated sen-
ratio, the effective shift of the Dirac voltage, strong absorption of sors. Some of the sensors involved the label-free electrical detection
the surface acoustic waves on a wide frequency range, and the of DNA hybridization. But, mostly the detection of DNA would
Hall Effect. The ability to display both metallic and semiconductive be done using biomolecular enzymes like ssDNA, RNA, aptamers
behavior as a single material allowed its extensive use in thin-film conjugated with graphene molecules [149–152]. The differences
transistors. It can show large on device currents at very low voltages between these sensors lies in their limit of detection (LOD) and the
[128,129]. range between which they could perform. One study [153] involved
the use of chemically reduced graphene oxide (CrGO) in a modified
4. Electrochemical sensors glassy carbon electrode (GCE) for the detection of four free bases of
DNA concurrently, which showed better results than just graphene-
Several reasons like a wide range of electrochemical potential, modified GCE. This establishment helped in the detection of the
fast electron transfer rate and high redox peaks with linear cathodic four bases for both single and double stranded DNA without the
and anodic currents have made graphene and its oxidized form (GO) requirement of a pre-hydrolysis step.
useful as electrochemical sensors for some time. Another significant aspect of graphene-based electrochemical
As mentioned in the earlier sections, with the modifications sensing, due to the fast electron transfer rate and high electro-
done on graphene sheets with methods like electrodeposition, catalytic capability of graphene, includes the detection of smaller
polymerization, electrochemical doping, etc., different composite biomolecules like uric acid, ascorbic acid and dopamine. The impor-
materials were developed for electrochemical sensing purposes. tance of the concentration of dopamine in the human body caused
Due to its high detection capability, graphene serves as an excel- researchers to work on it in the presence of other acids. Most of
lent molecule for combining with redox enzymes on the electrode the work exhibits the graphene-modified GCE [111,154–156]. Even
Fig. 6. (a) One-step approach to the formation of an H2 O2 sensor with PEDOT: PSS and AuNP and rGO. (b) Functionalization of the formed nanocomposite with HRP for
detection purposes [163].
Table 5
Summary of the graphene based electrochemical sensors depicting the differences between the responses concerning the materials and techniques used to develop the
sensors.
Material (with graphene) Technique Linear Range (␮M) Limit of Detection (␮M) Ref.
Copper Hummer’s method 0–4.5 0.5 [142]

Nickel oxide Hummer’s method 0.0005–3000 1.73 [45]
Zinc oxide Electro-deposition 0.02– 22.48 0.02 [160]
Carbon Nano-spheres Screen printing 0.05– 6 0.02 [148]
Cerium oxide Oxidation 12– 7200 4 [146]
though some of the developed sensors depicted a prominent lin- graphene-based sensors have proved to be an excellent candidate
ear range and LOD, the stability of the responses degraded with for strain-sensing applications. The advantage of using graphene
time. Due to the higher electron mobility and the wide electrical over other conductive material for strain sensing lies in the gen-
window of graphene, it is largely considered for the detection of eration of a pseudo-magnetic field due to the shift in the Dirac
biomolecules [157]. Graphene Field-Effect Transistors (GFETs), in cones and reduction of the Fermi velocity. The usefulness of this
recent years, have been successful as a bio-sensing device reducing magnetic field lies in its implementation to determine the change
the fabrication cost and response time due to their high sensi- in electronic structure during strain. The gauge factor (G.F.) is an
tivity. There is an increase in the gate current of GFETs on the important parameter which is used to determine the efficiency of
introduction of any biomolecule, causing a change in drain cur- fabricated strain sensors. It calculates the electric shift based on
rent. The Debye length and proper functionalization of the receptor mechanical deformations. This is because, as the graphene-based
with a single layer of graphene for specific detection of the tar- sensors involve different materials amalgamated to fabricate them,
geted molecules are the two parameters critically analyzed for the change in unit resistance to the change in unit length caused by
GFETs during bio-sensing applications. Detection of hydrogen per- the strain decides the amount of strain to be taken into account
oxide (H2 O2 ) with graphene-based sensors is another area where for the material. Some of the strain sensors with high G.F. use
researchers have focused in recent years. Graphene in its intrinsic graphene composites [164,165]. The amount of relative strain is
and N-doped (N-graphene) forms have shown excellent electrocat- more when applied parallel to the C C bonds compared to its appli-
alytic response towards H2 O2 [158–162]. The N-graphene form has cation perpendicular to the C C bonds due to a higher increase in
shown a better response due to the presence of nitrogen and oxy- the band gap. A lot of research groups work on developing graphene
gen functional groups along with structural defects. Fig. 6 shows films on polymer substrates like polydimethylsiloxane (PDMS),
a pictorial description of work done on the detection of H2 O2 by Polyethylene terephthalate (PET), Polyimide (PI) [166–168], getting
a one-step approach [163]. A nanocomposite was formed by mix- a piezo-resistive effect by causing a non-monotonic change in the
ing poly (3, 4-ethylenedioxythiophene) - poly (styrene sulfonate) electrical resistance with the applied strain. Fig. 7(a)–(c) show three
(PEDOT: PSS) with gold nanoparticles and reduced graphene oxide. different types of strain sensors developed with PDMS, PET, and PI
The nanocomposite was assembled to the electrode after being done with photolithography, drop-casting, and thermal annealing
functionalized with horseradish peroxide (HRP) for the detection of processes respectively.
H2 O2 . The sensor showed a high sensitivity of 677 ␮A mM−1 cm−2 Strain sensors, other than being used as pressure sensors, have
with a linear range and LOF of 5–400 ␮M and 0.08 ␮M respectively. been employed for different applications like healthcare devices
Table 5 shown below addresses some of the techniques used to where they have been attached to the gloves, skin and organs to
develop the graphene-based electrochemical sensors along with monitor physiological parameters. The changes in the G.F., elec-
their linear range and limit of detection. trical conductivity, and relative strain have been reported up to
269, 2200 S/cm and 540% respectively. Another work involved the
formation of a strain sensor to use it as a sound-signal acquisi-
5. Strain sensors
tion and recognition device [169–176]. The sensor was designed on
fabric (GWF) by weaving graphene with PDMS. The sensor patch
Even though strain sensors with different materials have been
was placed on the muscle of a throat to analyze the change in
formulated and developed for a significant amount of time, the
Fig. 7. (a) PDMS-based strain sensor developed with graphene on Ni/Si/SiO2 film [166]. (b) Flexible graphene-PET strain sensor developed by drop-casting graphene oxide
film to laser write the interdigitate circuit [167]. (c) Development of a reduced graphene oxide/polyimide nanocomposite to form strain sensors by mixing, freezing and
thermal annealing with poly (amic acid) [168].
Fig. 8. Schematic diagram of the formation of stretchable graphene nano-papers [178].
Table 6
Summary of graphene-based strain sensors based on the materials and technique used to differentiate between the gauge factor and maximum strain.
Material (with graphene) Technique Gauge factor Max. Ref.
PDMS CVD 14 7.1 [166]

PET Drop casting 9.49 7.5 [167]
PDMS CVD 106̂ 7 [24]
Nano-graphene films RPECVD 300 0.37 [176]
Graphene oxide Hummer’s method 7.1 100 [178]
the electrical resistance with the movement of the throat mus- pled graphene and nano-cellulose fibril were mixed at a weight
cles. After the response of the sensor for every English phoneme ratio of 1:1 on a polycarbonate membrane. Following filtration of
was analyzed to differentiate its output, different words were tried the embedded nanocomposite, the thin film was peeled off and
to validate the developed sensor further. There were other stud- impregnated with PDMS to develop the stretchable nano-papers.
ies reported on GWF where even a G.F. factor up to ∼105 was The movement of the fingers caused a 3D movement of the sen-
achieved. Graphene, in the form of nano-papers, were also used to sor leading to a maximum strain exceeding 50%. Table 6 depicts
develop strain sensors [24,177,178]. The sensor patch was used to the some of the techniques used to develop the strain sensors with
detect human movements. Fig. 8 gives the schematic diagram of the graphene electrodes along with their strain percent and gauge fac-
fabrication steps of the nano-cellulose based sensor patch. Crum- tor.
6. Electrical sensors make them popular for these applications. The physical sensing
includes the employment of graphene electrodes as phototransis-
The use of graphene in electrical and electronic applications has tors and thermal transistors. The unimpeded transmission of the
been comparatively minor compared to the preceding explained carriers in GFETs as a result of the very small band gap makes
applications. Graphene has been largely employed as transistors for graphene a very popular choice for phototransistors [208,209].
biomolecular applications. Other uses of graphene-based electrical Due to the high mobility of the carriers, ultrafast photodetectors
sensors include temperature sensing, photodetectors, RF applica- have also been fabricated with graphene with a varied number of
tions [179–182], etc. Graphene has been utilized in the form of layers. Even though the highest photo-responsivity has not been
nanoribbons, nanowires and other forms of nanoparticle arrays. very high for the graphene photodetectors, moderately high val-
Among the photodetectors, the GFETs cover the terahertz, IR, ues of ∼1 × 107 A W−1 , response rate values higher than 20 GHz
visible and UV ranges [88,183–185]. Graphene transistors are fabri- and optical data links of 12 Gbit/sec has been achieved. The ther-
cated on flexible substrates (PI, flexible glass, Kapton, Polyethylene mal transistors developed with graphene sometimes contain an
Napthalate) that are attached to rigid substrates via or not via additive layer to increase its stability while protecting the sens-
gelling/interface material (SiO2 , PDMS) [186–190]. The flexible sub- ing surface from oxidation and water. Some scientists have also
strates are introduced, through spin coating followed by a baking tried to amalgamate the properties of graphene sensors to develop
process, into the rigid substrates. The gate and metal contacts of Field-Effect Transistors (FETs) having other prominent mechanical
varying compositions (Au (100 nm) / Ti (10 nm), Au (38 nm) / Ti features like high strain-sensing capabilities [210–212].
(2 nm), Au, Al (40 nm) / Ni (50 nm) /Au (300 nm), Cr (1 nm) / Au The electrical sensing fields using GFETs include the employ-
(60%) – Pd (40%) alloy (20 nm)) [38–42] are made by employing one ment of these sensors for studying different metallic ion in solution.
of the following processes: E-beam, photolithography, and inkjet Some of the heavy metallic ions like cadmium, lead, mercury have
printing techniques followed by plasma etching in an atmosphere been detected at low concentrations with the use of GFETs. The
of O2 at specific conditions (300 W/5 mbar/5 min) at room temper- detectable concentration ranges from a few nano molar ranges as
ature. The graphene is washed and transferred from CVD or other shown in the table below. Other than the heavy ions, some of the
processes (inkjet printing) over the transistor’s length over the gate commonly used ions like calcium, potassium, hydrogen have also
dielectric (HfO2 , nanoscale polyimide, Al2 O3 ). The graphene forms been detected by these sensors. The detection of the ions using
the channel also, in the process covering the contact materials. The these sensors takes place by non-covalent functionalization of the
fabricated graphene transistor of the varying gate length, channel sensing surface of the electrodes with the analyte ions. The other
width, and channel length is finally removed by mechanical peel- applications of GFETs in chemical sensing include the sensing of pH
ing off the flexible substrate or dissolving a flexible substrate by and different gasses like ammonia, nitrogen dioxide, and other inor-
using acetone. Fig. 9 shows the schematic diagram of the fabrication ganic gases. Graphene has been grown on different substrates like
of graphene transistors in different views [72]. The combination SiC, poly (ethylene 2, 6-naphthalenedicarboxylate), etc. and trans-
of nanowire field-effect transistors (NW-FETs) and GFETs inter- ferred using mechanical transfer on flexible substrates. Some of
face well with the electrogenic cells resulting in a highly sensitive the studies regarding gas sensing as shown below exhibits such
response towards cell membranes [179]. very low detectable concentrations as ppb at different gate volt-
Other uses of graphene in electrical sensors involve its uses ages. Table 8 gives an overview of some of the selected work done
in lithium-ion batteries, photodetectors, inverters and optoelec- on chemical sensing using GFETs. It gives the type of substrate used
tronics. The inclusion of graphene in batteries is done by forming to grow graphene, the detected material, the range of gate voltages
clusters with lithium or mainly by forming hybrids with other com- and the lowest detectable concentration.
pounds. A range of compounds like Mn3 O4 , Fe3 O4 and was mixed
with modified graphene like rGO sheets and graphene nanosheets
respectively in the batteries [191–193]. The hybrid materials cre- 7. Challenges with the current sensors
ated with different compounds help with a quicker charging and
discharging capability than conventional lithium-ion batteries. Although there has been a lot of research work done and going
Pure graphene was also used where it was doped with materials on with sensors based on graphene and its different forms, there
like boron and nitrogen to increase the power, energy storage and are still some challenges that need to be addressed at the grass-
discharging capacity of the batteries. Other advantages of includ- roots level. The fabrication of graphene is a complex and expensive
ing graphene to develop batteries are its low-cost and light weight. process. It requires a significant amount of time to generate high-
Graphene has also been used largely in photodetection applications quality graphene. Techniques to generate low-cost graphene are
like optical modulators, plasmonic devices, etc. [185,194–197]. One yet to be commercialized. Some of the catalysts used during the
of the important goals of researchers developing photodetectors is growth of graphene increase its toxicity after its production [227].
the ability to generate a material covering most of the spectrum. This makes it difficult to use for biomolecular detection and other
Two of the advantages of using graphene in photo-sensing devices biomedical applications. It can also be addressed during its growth.
is its ability to detect right across a large spectrum along with The nanocomposites formed with graphene to develop or modify
its high sensitivity towards any polarized angle. Due to the excel- the electrode surfaces affect the intrinsic properties of the material.
lent transport properties of graphene, a high speed, even up to 10 For example, the electrical conductivity of the composite decreases
GB/sec, with a very high bandwidth of >500 GHz has been achieved. drastically (in terms of 103 ) compared to graphene. This could be
It is also the only material that could be used to develop photodetec- crucial in applications demanding highly conductive electrodes.
tors which are CMOS compatible and able to achieve their operation Secondly, the thermal stability also reduces in the case of nanocom-
over all the fibre-optic communication bands [198–200]. Table 7 posites due to a weaker interaction between the graphene and
gives a summary of some of the graphene-based transistors with matrix compared to the pure form of graphene. These effects can be
their achieved maximum strain and electron mobility [201]. tackled by treating the formed composites with an extra step like
There has been prominent work done on the utilization of chemical or thermal reduction [228,229], but this would demand an
graphene-based electrical sensors for biomolecular, physical and extra step which could be convoluted in the case of multi-layered
chemical sensing [207]. The simplicity in the design, easy of mass structures. Also, the homogeneity of graphene in oxide forms is
production and the capability to capture and amplify signals are almost impossible in the composites due to its poor dispersion.
some of the advantages of graphene-based electrical sensors which This leads to the addition of an extra step like the ball-mill mixing
Fig. 9. Graphene transistors on flexible substrate shown in 3-D (a), Optical (b), cross-sectional (c) and AFM (d) images [39].
Table 7
Summary of graphene-based electrical sensors based on the materials and technique used to compromise between the maximum strain and electron mobility [201].
Material (with graphene) Technique Electron mobility 2 V−1 s−1 ) Max. Strain (%) Ref.
Al2 O3 CVD 190 0.62 [202]

Ion gel Aerosol jet printing 422 5 [203]
Graphene oxide Langmuir− 4.1 3.5 [204]
PMMA Electron -beam lithography 8 1.2 [205]
Boron nitride Mechanical exfoliation 60000 – [206]
Table 8
Comparison between the different parameters for the chemical sensing done by GFETs.
Type of substrate Detected material Gate voltage (V) Lowest detectable concentration/ range of detection Reference
6H-SiC NO2 10 ppb

Cu NH3 ,CO2 >1 30 ppm, 4000 ppm [213]
N-type silicon wafer NO2 ,NH3 −5 - 5 10 ppm, [214]
Cu NH3 15 50 ppm [215]
SiO2 /Si H2 0 1 ppm [216]
SiO2 layer NO2 ,2 0 550 ppb [128]
SiO2, poly(ethylene 2,6-naphthalenedicarboxylate) pH >0.5 Neutral to Acidic [217]
SiC/silicon pH −1– 1 4.3 - 7 [218]
SiO2 layer (Degenerately doped silicon wafer) pH −0.1–0.1 4 – 9.3 [219]
SiO2 /Si pH −0.8 –0.8 6–9 [220]
Scotch tape, SiO2 layer pH Gate free chem-resistor 4–10 [221]
Silicone rubber/Glass Pb2+ 0–1 0.02 g/L [222]
Glass pH −0.2– 0.4 3–10 [223]
SiO2 / adhesive tape K+ −0.3 – 0.3 10 nM– 1.0 mM [224]
SiO2 Hg2+ −20–20 1 nM [225]
PDMS Ca2+ –0.6–0.6 1 ␮M [226]
process to increase the rate of dispersion [230]. The vulnerability of 8. Conclusion

graphene to be oxidized in oxidative environments is another major
disadvantage to be dealt with. This makes it extremely difficult to Some of the significant research work on graphene-based sen-
utilize graphene in its pure form. Another disadvantage of obtain- sors in different fields had been presented in this review paper. The
ing pure graphene lies in the amount of raw materials required to conversion of graphene in different forms increases the dynam-
generate it. For example, when graphene oxide (GO) is used to pro- icity of its properties, causing an expansion in its applications.
duce rGO, the chemical reduction causes a huge mass loss leading There has been some research reported by different groups on com-
to very small amounts of generated samples [231]. plete graphene-based sensing systems [232–234]. Their detection
methodologies include mostly electrochemical sensing techniques.
The data collected by the sensors are sent to the monitoring unit
using different wireless protocols. Some of the electrochemical tages to graphene over CNTs and other allotropes of carbon. Firstly,
applications include bacteria detection on tooth enamel, where they can be used in the purest form to develop the electrodes of
graphene was printed onto a water-soluble silk forming a sensing a sensor. Secondly, the cost of production of pure graphene is get-
platform. This system was used for selective bio-detection of bacte- ting less than other materials [243]. They are also advantageous
rial cells. The wireless conditioning circuit included a single-layer for energy-storage applications like the production of fuel cells,
LC resonant circuit with a parallel resistive graphene monolayer. lithium ion batteries and ultra-capacitors due to their ability to
Another electrochemical application with graphene-based wire- be charged and discharged under intercalation potentials. Differ-
less sensors involves transparent gas sensors developed with an ent lithium-ion batteries and fuel cells have used graphene in the
amalgamation of graphene and silver nanowires. Here, the wireless pure form or mixed it with other materials to increase the stor-
system contained a Bluetooth system embedded with an antenna. age capacity. Another advantageous characteristic of graphene its
Electrical sensors developed with graphene includes graphene ability to display of half-integer quantum Hall effect at the speed
varactors which were fabricated with a combination of a metal- of light even at room temperature. The charge density of graphene
insulator-graphene structure having a capacitance varying with can be controlled by the gate electrode, thus providing an ambi-
the charge concentration as a result of the quantum capacitance polar electric field effect having excellent electrode kinetics due to
effect. These devices along with an embedded LC oscillator cir- the high mobility of the carriers. It has the ability to carry super
cuit are very useful for wireless readout purposes. The quantum current because of the continuous charge carries which are of high
capacitance of graphene sensors has been put into use in other crystal quality, making light travel thousands of inter-atomic dis-
wireless sensing systems [235] even for simple detection of humid- tances without any scattering [244]. The graphene-based sensors
ity concentrations. The results obtained from the experimental are also advantageous for bio-sensing purposes for two reasons.
values with quantum capacitance have been cross-checked with Firstly, it has a high density edge plane and can act as a nano-
capacitance-voltage measurements to validate the former’s use in connector between the analyte and the electrodes. Secondly, the
sensing systems. Other wireless protocols involved in complete availability of their two-dimensional electronic states on the sur-
graphene based sensors involve the Wireless Integrated Sensing face makes them accessible by tunneling techniques. This leads to
Platform [236]. This system used both analog and digital wire- the mediator-less direct transfer of electrons between the enzymes
less remote transmission principles while eliminating the use of and the electrode surface. The flexibility of graphene sheets is also
any wire or battery operations. This system was combined with higher than other allotropes of carbon like graphite, thus helping to
graphene-based gas sensor modules to detect NH3 and CO gases. form flexible electronic devices. Strain sensors with high GF can be
Another wireless protocol commonly used in complete sensing sys- developed using graphene, whose performance in terms of resis-
tems is the Radio-Frequency Identification Tag (RFID) combined tivity remains fairly constant even after a large number of bending
with graphene-based sensing systems. The entire system consisted cycles. Even though a lot of research has been done on these sen-
of platinum-decorated reduced graphene oxide attached to a RFID sors, there are still some limitations which need to be addressed
sensor tag and an RFID reader antenna connected to a network and rectified to improve the efficiency in the utilization of these
analyzer. The sensing system was used to detect hydrogen gas at sensors on a commercial basis. Some of the limitations related to
low concentrations [237]. The Zigbee standard is another wireless different graphene-based sensors are given in Table 9. It is seen
protocol involved with graphene-based sensing systems. These are from the table there is still a lot to be done to address the funda-
used for the measurement of different pH and glucose concentra- mentals characteristics of this material to make it more efficient to
tions. The sensed data were transmitted from the sensor to the XBee develop graphene-based sensors.
router via the XBee coordinator. This data was then interpreted
using LABVIEW to extract significat information.
Apart from these sensing systems, in order to increase the 9. Future opportunities
usability of graphene-based sensors, categorization can be done
based on their strengths and limitations. Some of the advantages of Although there have been some drawbacks of graphene and
graphene lie in the characteristics associated with its physicochem- its sensor-based applications as mentioned in the previous sec-
ical structure. The sp2 hybridized carbon atoms of the graphene tion, graphene can still be considered one of the most promising
structure makes it highly conductive due to the absence of an elec- material in the last few decades that have been synthesized in
tron in the outermost shell. The electrical conductivity of graphene the laboratory and employed for various applications. The number
is around 60 times more than that of CNTs which makes it a favor- of potential applications using graphene sensors can be increased
able choice to form the nanocomposite-based electrodes of the by converting more of the graphene-based sensors into sensing
sensors. The very low bad gap between the valence and the conduc- systems. The sensors can be embedded to form wearable sens-
tion band is another advantage which leads to the employment of ing systems for ubiquitous monitoring of physiological parameters
these materials in supercapacitors [238–241]. There are four dis- and other chronic diseases. The sensors attached to the body
tinct advantages of graphene, which makes it a favorable choice should be made sturdier to sustain wear and tear for a long
for electrochemical sensors. Firstly, it exhibits a high surface area, time. This can be attained by modifying the physical and chemi-
thus having a higher and more uniform number of electrochem- cal characteristics of the substrates that are used to develop the
ically active sites than that of other similar electrode materials. sensors. Many more day-to-day applications can be addressed by
Secondly, the availability of oxygen-containing groups in its struc- increasing the selectivity and specificity of graphene sensors. The
ture greatly influences the electrochemical performances in terms response of graphene electrodes to target analytes and molecules
of electron transfer rates. Thirdly, the presence of the oxygen groups should be increased while decreasing their responses to interfer-
also influences the adsorption and desorption of molecules taking ing molecules. Functionalization of graphene electrodes should be
place during the electrochemical reaction. Fourthly, the electro- utilized more, with capture agents for specific target molecules.
chemical modification can be done in covalent and non-covalent More focus should be given on non-invasive, label-free detection
ways to functionalize the electrodes of the sensors with additional of different biomolecules. The fabrication of the graphene sensing
operations. Another big advantage of using graphene is the absence systems should also be enhanced to produce low-cost, reusable
of heterogeneous materials during its production with methods sensors. One way to improve the quality of fabrication techniques is
like CVD, unlike CNTs which contain carbon-containing gases with to use devices operating with less complexity and low input power.
metallic nanoparticles as catalysts [242]. This provides two advan- Another way to develop the fabrication procedure is to develop
Table 9
Limitations of graphene as showcased in various research.
Sl. No. Limitations Reference
1. The maximum photo-responsivity of graphene photodetectors is low. This is [245]

due to the small detection area of the graphene sheets and the very short
photo-generated carrier lifetime.
2. It is susceptible to oxidative environments. Thus, it cannot be used as a [246]
catalyst in redox reactions.
3. Point defects are present in graphene due to its sp2 hybridizing property [247]
which results in the formation of various non-hexagonal structures. This alters
the electro-mechanical properties of the resultant electrodes of the sensors.
4. Even though a lot of graphene-based strain sensors have been developed in
the laboratory environment, the stretch-ability is still insufficient due to the
defect density in its structure.
5. The presence of multilayers in graphene sheets results in interlayer sliding,
leading to a difference in crack densities.
6. Defects occur in graphene’s structure during its interaction with metallic [248]
substrates.
7. There are oxides in the surface of graphene which affect the electronic and [249]
chemical properties.
8. There are unknown cytotoxic limitations in graphene sensors which limit their
usage in bio-sensing applications.
9. A lot of parasitic effects are present in graphene which influences the response [250]
of the graphene-based sensors.
10. The formation of different compounds with graphene changes its structural [251]
composition on which when an external load is applied, producing fracture
lines, and increasing the number of dangling bonds in its structure.
Fig. 10. An overview of the potential applications and marketing areas of graphene in the upcoming years [252].
sensors with consistent performance in terms of efficiency. This ties of the material, thus reducing the overall efficiency. More work
can be achieved by not only addressing the performance of the based on the diffusion processes and surfactants associated with
sensors, but also the signal conditioning embedded with the sen- graphene has to be done for its uniform dispersion in the differ-
sor. Another approach to reduce the production cost is to fabricate ent matrixes to form nanocomposites. The biocompatibility of the
multi-functional sensors, where the different parameters can be graphene sensors should be exploited more by replacing the non-
addressed with a single sensing system. The signal-to-noise ratio biocompatible commercial sensors that are currently available in
of graphene sensing systems should be looked into to maximize the market. Graphene has always had a very bright side in its utiliza-
the accumulation of useful information. When developing sensors, tion in commercial fields for various applications since its synthesis
the structure of graphene is sometimes modified by separating the in the laboratory over the last two decades. The global market for
individual sheets. This changes the electrical and thermal proper- graphene is estimated to rise to 250 million USD by 2020 with an
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[244] D.A. Brownson, C.E. Banks, Graphene electrochemistry: an overview of and Doctor of Engineering degree from Kanazawa Uni-
potential applications, Analyst 135 (2010) 2768–2778. versity, Japan. Currently he is working as a Professor of
[245] Y. Liu, Q. Xia, J. He, Z. Liu, Direct observation of high photoresponsivity in Mechanical/Electronics Engineering with the Department
pure graphene photodetectors, Nanoscale Res. Lett. 12 (2017) 93. of Engineering, Macquarie University, New South Wales,
[246] Advantages and Disadvantages of Graphene. Australia. He is the Program Leader of the Mechatron-
[247] S.-M. Lee, J.-H. Kim, J.-H. Ahn, Graphene as a flexible electronic material: ics Engineering Degree Program. He has over 26 years
mechanical limitations by defect formation and efforts to overcome, Mater. of teaching and research experiences. His fields of inter-
Today 18 (2015) 336–344. est include Smart Sensors and Sensing Technology, Wireless Sensor Networks,
[248] S. Karoui, H. Amara, C. Bichara, F. Ducastelle, Nickel-assisted healing of Instrumentation and Measurements, Internet of Things, Environmental Measure-
defective graphene, ACS Nano 4 (2010) 6114–6120. ments, Electromagnetics, Control Engineering, Mechatronics, Magnetic Bearing,
[249] D.R. Dreyer, S. Park, C.W. Bielawski, R.S. Ruoff, The chemistry of graphene Fault Current Limiter, Electrical Machines and numerical field calculation etc. He
oxide, Chem. Soc. Rev. 39 (2010) 228–240. has authored/co-authored over 400 papers in different international journals, con-
[250] Y. Wu, Y.-m. Lin, A.A. Bol, K.A. Jenkins, F. Xia, D.B. Farmer, et al., ferences and book chapter. He has edited fifteen conference proceedings. He has
High-frequency, scaled graphene transistors on diamond-like carbon, also edited seventeen special issues of international journals as lead guest editor
Nature 472 (2011) 74–78. and thirty books with Springer-Verlag. He was awarded numerous awards through-
[251] H.C. Schniepp, J.-L. Li, M.J. McAllister, H. Sai, M. Herrera-Alonso, D.H. out his career and attracted over US$3.0 M on different research projects. He has
Adamson, et al., Functionalized single graphene sheets derived from delivered 296 seminars including keynote, tutorial, invited and special seminars.
splitting graphite oxide, J. Phys. Chem. B 110 (2006) 8535–8539. He is a Fellow of IEEE (USA), a Fellow of IET (UK) and a Fellow of IETE (India). He is
[252] Graphene Market Trends. Available on http://www.strategyr.com/ a Topical Editor of IEEE Sensors Journal, and an Associate Editor IEEE Transactions
MarketResearch/Graphene Market Trends.asp. Last accessed on 28th on Instrumentation and Measurements. He is in the editorial board of e-Journal on
November, 2017. Non-Destructive Testing, Sensors and Transducers, Transactions on Systems, Sig-
[253] Graphene Market Overview. Available on https://www. nals and Devices (TSSD). He is the co-Editor-in-chief of the International Journal on
alliedmarketresearch.com/graphene-market. Last accessed on 28th Smart Sensing and Intelligent Systems (www.s2is.org). He was the Technical Pro-
November, 2017. gram Chair of ICARA 2004, ICARA 2006, ICARA 2009 and IEEE I2MTC 2016. He was
[254] Graphene Market Reports. Available on https://www.graphene-info.com/ the General chair/co-chair of ICST 2005, ICST 2007, IEEE ROSE 2007, IEEE EPSA 2008,
tags/market-reports. Last accessed on 28th November, 2017. ICST 2008, IEEE Sensors 2008, ICST 2010, IEEE Sensors 2010, ICST 2011, ICST 2012,
ICST 2013, ICST 2014, ICST 2015 and ICST 2016. He has organized the IEEE Sensors
Biographies conference 2009 at Christchurch, New Zealand during October 25 to 28, 2009 as the
General Chair. He is currently organizing the 11th ICST in Sydney, Australia dur-
ing December 4–6, 2017, (http://www.cvent.com/d/nvqbb9). He is the Ex-Chair of
the IEEE Instrumentation and Measurement Society New Zealand Chapter. He is a
Mr. Anindya Nag has completed Bachelor of Technol- Distinguished Lecturer of IEEE Sensors Council from 2017-2019.
ogy from WEST BENGAL UNIVERSITY OF TECHNOLOGY
in 2013 and Master of Engineering at Massey University,
Palmerston North, New Zealand in June 2015. His research
interests are in the area of Smart Sensors and Sensing
Technology for home and environmental monitoring. He
is currently pursuing PhD in Engineering at Macquarie
University, Sydney, Australia and is working on Printed
Flexible Sensors for Human Wellness.

Graphene Based Smart Sensors

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Sensors and Actuators A 270 (2018) 177–194

Contents lists available at ScienceDirect

Sensors and Actuators A: Physical

Graphene and its sensor-based applications: A review

Fig. 1. Different forms (0D, 1D and 3D) of modiﬁed graphene [11].

Graphene ∼106 120 Non-linear up to 1% [24]

Carbon Nanotubes 12.1 410 Linear [29]

Silver 2-14 70 Linear up to 40% [35]

Electrode material Limit of Detection Sensitivity Linear range References

Silver 29.2 ␮M 0.0266 ␮A cm−2 ␮M−1 0.1–3.1 mM [52]

Technique Gas source/reducing agent Temperature (◦ C) Substrate References

SWP-CVD CH4 :Ar:H2 300 − 400 Cu, Al [75]

of time. Sulfur-laced reducing agent (NaHSO3 , Na2 S.9H2 0, SO2 ) in a are:∂1 = 2

Zigzag 6.395 4.184 1.040 0.213 1.441

Copper Hummer’s method 0–4.5 0.5 [142]

Fig. 8. Schematic diagram of the formation of stretchable graphene nano-papers [178].

Material (with graphene) Technique Gauge factor Max. Ref.

PDMS CVD 14 7.1 [166]

Al2 O3 CVD 190 0.62 [202]

6H-SiC NO2 10 ppb

process to increase the rate of dispersion [230]. The vulnerability of 8. Conclusion

Sl. No. Limitations Reference

1. The maximum photo-responsivity of graphene photodetectors is low. This is [245]

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