Ceramics International 47 (2021) 16367–16384

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Ceramics International
journal homepage: www.elsevier.com/locate/ceramint

Review article

Review of recent progress on graphene-based composite gas sensors

Chenyang Wang a, b, Yanyan Wang a, b, *, Zhi Yang c, Nantao Hu c
a
School of Optoelectronic Science and Engineering & Collaborative Innovation Center of Suzhou Nano Science and Technology, Soochow University, Suzhou, 215006, PR
China
b
Key Lab of Advanced Optical Manufacturing Technologies of Jiangsu Province & Key Lab of Modern Optical Technologies of Education Ministry of China, Soochow
University, Suzhou, 215006, PR China
c
Key Laboratory of Thin Film and Microfabrication (Ministry of Education), Department of Micro/Nano Electronics, School of Electronic Information and Electrical
Engineering, Shanghai Jiao Tong University, Shanghai, 200240, PR China

A R T I C L E I N F O A B S T R A C T

Keywords: Development of gas sensors for detecting toxic, harmful, flammable, and explosive gases has always been very
Graphene popular research direction. Graphene is considered potential chemi-resistive gas sensing material owing to its
Gas sensor high specific surface area and good conductivity. Recent studies have shown that graphene-based gas sensors
Metal
doped with metals, polymers, and metal oxides have good sensitivity, selectivity, and repeatability. Moreover,
Metal oxide
Polymer
they are superior to traditional gas sensors. In this review, sensing mechanism of such composite sensors is
Sensing introduced. In addition, research status on various sensors is discussed, and their advantages and disadvantages
are summarized. Possible improvement methods are proposed as well. Finally, several common problems
characteristic of graphene-based gas sensors are described, together with some critical ideas for improving their
performance.

1. Introduction causing harm to people and the environment alike [8–12].

In recent years, with the rapid industrial development, environ­
mental pollution has become an increasingly serious problem. The
research and development on high-performance gas sensors as well as
the realization of real-time, rapid, and accurate monitoring of toxic and
harmful gases at room temperature have become a hot spot in current
research topics. In many countries, the combustion of fossil fuels leads to
the emission of harmful gases, such as nitrogen oxides, which destroy
the environmental balance [1]. Therefore, the detection of NOx, and
especially of NO2, has triggered a considerable interest, since it is not
only harmful for the respiratory system of human beings, animals, and
plants, but is also responsible for acid rain formation [2–5]. Hydrogen
sulfide is another poisonous and harmful gas, which is easily produced
during the production process of oil and natural gas. This compound is
highly dangerous for the human body [6]. NH3 is an irritant and cor­
rosive gas, which causes great harm to the human body and the envi­
ronment. Low concentrations of NH3 in air or liquid can cause severe
irritations and cough when they get in contact with the skin or the eyes
[7]. Therefore, it is of great social significance to develop
highly-sensitive sensors to monitor these gases and prevent them from
Currently, most gas sensors are based on metals [13,14], polymers
[15], and metal oxides [16–18]. However, their sensitivity is not high
enough, and their gas selectivity is limited. Their power consumption
and temperature-dependency are significantly large, and their safety is
not guaranteed. Since graphene-based gas sensors can limit the short­
comings of traditional sensors and have characteristics that traditional
sensors do not possess, they have become the main hot topic for
gas-sensor research. Graphene is a two-dimensional material with a
hexagonal honeycomb lattice composed of carbon atoms and a SP2
hybrid orbital. Owing to its high specific surface area of 2600 m2/g and
low carrier thermal vibration noise, graphene has unique advantages in
gas sensing. The honeycomb structure of a single carbon layer exposes
all carbon atoms to the environment, providing the maximum contact
area between gas and graphene. Its resistance varies greatly with the
change in carrier concentration at a low carrier noise. The unique
structure and excellent properties of graphene compensate for the
shortcomings of other gas sensing materials: for this reason, graphene
has huge potential in the field of gas sensors. Theoretically, gas detection
performed with graphene sensors can reach the single-molecule level.
After K. S. Novoselov [19] found that graphene has an excellent

* Corresponding author. School of Optoelectronic Science and Engineering & Collaborative Innovation Center of Suzhou Nano Science and Technology, Soochow
University, Suzhou, 215006, PR China.
E-mail address: yywang@suda.edu.cn (Y. Wang).

https://doi.org/10.1016/j.ceramint.2021.02.144
Received 28 September 2020; Received in revised form 29 January 2021; Accepted 16 February 2021
Available online 19 February 2021
0272-8842/© 2021 Elsevier Ltd and Techna Group S.r.l. All rights reserved.
C. Wang et al.
electrical response to gas molecules, R. S. Ruoff [20], N. Koratkar [21,
22], R. B. Kaner [23,24], and other research groups have conducted
extensive research on the gas sensing properties of graphene.
Graphene-based sensors are usually based on a conductive network
constructed via a series of graphene sheets, which correspond to the
sensing structure of the device. However, such sheets can easily arrange
in a dense structure during the stacking process to form a conductive
network. This hinders the gas molecule motion, causing them to stick
together, which is unfavorable for the full contact between the graphene
sheets and gas molecules in the conductive network. In order to further
improve the gas sensing performance of the sensor, it is necessary to
design and control the micro-nanostructure of the graphene conductive
network.
In addition, graphene and its derivatives, such as original graphene
(G), graphene oxide (GO), and reduced graphene oxide (rGO), have been
widely investigated owing to their excellent properties [25–34]. rGO is a
form of graphene [35–44], which can be obtained via the reduction of
graphene oxide. rGO is not only easy to fabricate, but also cheap to be
manufactured in a large-scale production. Due to such unique functions
and gas sensing properties, rGO-based gas sensors have attracted a huge
interest among researchers [45–49]. Moreover, researchers have
explored graphene/nanomaterial composites, especially metals, con­
ducting polymers, and metal oxides [50–53], to improve the perfor­
mance of such sensors. Therefore, in recent years, close attention has
been paid to graphene-based mixed structures [54–60]: gas sensors with
high sensitivity, selectivity, and repeatability, which work at room
temperature. In short, graphene-based gas sensors permit the develop­
ment of highly effective, low-cost sensors with a very simple
manufacturing method. These devices meet the requirements of several
gas-monitoring applications. In this review, the performance enhance­
ment mechanism obtained through doping graphene with different
materials is briefly summarized. The review then proceeds to analyze
gas sensors based on graphene doped with metals, polymers, and metal
oxides. Graphene-based gas sensors doped with metals, polymers, metal
oxides, and even mixed materials, such as metal-polymer, metal-metal
oxide, and polymer-metal oxide combinations, show excellent sensing
performance. These nanomaterials exhibit a good gas sensitivity and an
enhanced gas sensing performance. Finally, the application potential of
graphene-based composite sensors is described, and the prospects of
these composite sensors are discussed in detail.
2. Basic working mechanism
Both two-dimensional and three-dimensional graphene materials
have high electrical conductivity and large specific surface area. On the
one hand, gas molecules, both electron donors and acceptors, once
adsorbed onto the graphene surface, induce changes in the carrier
concentration around graphene, thus varying its resistance. On the other
hand, the huge surface area of graphene enables the adsorption of gas
molecules [61].
In the literature, many types of noble metals used in gas sensing
[62–68] have been reported, and these metal-based sensors show an
excellent sensing performance. Several metals exhibit a good adsorption
for gases, such as Pd in hydrogen sensing. Hydrogen sensors based on Pd
have been widely investigated. The performance of these devices can be
further enhanced by introducing graphene in their structure. Several
other metals can catalyze the decomposition of gases into active radicals
and enhance their combination with oxygen-containing functional
groups onto the surface of graphene [69], thus exhibiting a good
response to such gases. Graphene has a high specific surface area and
high mechanical strength, which provides an ideal support layer for Pd
in the H2 induction processes [70]. The direct charge transfer process
between the gas molecules and the graphene surface is the main
mechanism [69]. Different metals exhibit a catalytic effect when they
come in contact with different gases. When in coordination with gra­
phene, the sensor performance of the two-material composites is
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significantly increased.
Polymers are a type of porous macromolecular materials with a large
specific surface area [71], which can be used in the field of gas sensors
[72]. In recent years, many groups have fabricated graphene-based gas
sensors modified with polymers. Common substances, such as polyani­
line, polypyrrole, and polythiophene, not only have a high specific
surface area, but also exhibit special conductive properties. After com­
pounding with graphene, they form a π-π conjugation [73], which en­
dows the device with good gas sensing properties. Owing to the
synergistic effect between polymers and graphene, the sensing perfor­
mance of the obtained sensor is much higher than that of a pure polymer
or graphene sensor. Thus far, polymers used in gas sensors have been
widely investigated [74–78].
Metal oxides are materials with a large specific surface area, which
can easily adsorb gas molecules onto their surface: for this reason,
several investigations have focused on these materials for gas sensors.
Both metal oxides and graphene have a large specific surface area. Their
combination exhibits a large specific surface area, which offers
numerous active sites, and enables the gas to be adsorbed onto the
sensor surface. Moreover, graphite prevents metal-oxide agglomeration,
whereas metal oxides prevent graphene fossilization. The oxygen pre­
sent in the air acquires electrons from the oxides conduction band and
forms several adsorbed oxygen species, such as O−2 , O− , and O2− . At this
point, a depletion layer with low free-electron concentration forms on
the surface of the metal oxides, and the resistivity increases. Once the
sensor is exposed to the measured gas, the target gas captures electrons
from the conduction band and reacts with the oxygen molecules on the
surface of the sensor material. This results in a decrease of the conduc­
tivity of the whole sensor. In addition, most metal oxides are n-type
semiconductors, whereas graphene is a p-type semiconductor. The p-n
junction formed during the integration process of the two materials can
enhance the conductivity. This phenomenon can be explained via the p-
n heterostructure theory [79,80]. The Fermi energy level of metal oxides
is generally lower than that of graphene; for example, it is 4.8 eV for
SnO2 and 5.4 eV for rGO. Therefore, graphene, being an electron
acceptor, acquires electrons from the surface of the metal oxide, pushing
the Fermi energy of both materials to the same level. In this way, the
number of electrons on the surface and at the interface of the metal oxide
decreases, the potential barrier increases, the depletion layer broadens,
and the resistance of the whole sensor significantly changes. Therefore,
composites consisting of a metal oxide and graphene are excellent de­
vices for gas sensing. Several investigations have been devoted to the
study of metal oxide-based gas sensors [81–91].
Graphene-based gas sensors doped with two mixed nanomaterials
show an excellent sensing performance. Their sensing mechanism is
relatively complex. Three categories for such type of sensors exist:
metal-polymer mixed, metal-metal oxide mixed, and polymer-metal
oxide mixed. The sensing mechanism for composite sensors composed
of a metal and a polymer can be explained by the metal catalytic effect
and synergistic effect between the polymer and graphene. The whole
polymer/rGO system can be described as a semiconductor with p-type
characteristics. The main sensing mechanism for this type of sensor is
the electronic transmission with the metal. The sensing performance of
graphene-based composite sensors doped with a metal-metal oxide is
mainly determined by the individual characteristics of the metal oxide
and graphene, with the metal playing a catalytic role. More details can
be found in Section 3. The main sensing mechanism of graphene-based
composite sensors doped with a polymer-metal oxide can be explained
via the p-n heterostructure theory: the polymer/rGO system behaves as a
p-type semiconductor, whereas the metal oxide is a n-type semi­
conductor and thus provides the electrons. A p-n junction forms between
the polymer/rGO and metal oxide. For this reason, a composite sensor
doped with two materials retains the characteristics of each of its
components, while also overcoming their disadvantages. Further details
are provided in Section 6 of this review.
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3. Graphene-based gas sensors doped with metals
3.1. Sensors for H2 gas sensing
Being highly effective catalysts for hydrogen, both platinum and
palladium are commonly used to manufacture hydrogen sensors. How­
ever, when metals are treated as catalysts, the hydrogen absorption in­
creases the sensor volume, affecting its stability and leading to hysteresis
[92,93]. However, the porous structure of graphene allows this expan­
sion, mitigating the hysteresis effect. D. T. Phan et al. [94] reported a
graphene-based sensor doped with platinum for hydrogen detection.
They packaged Pd/G into a three-dimensional (3D) structure via the
hydrothermal method to improve the sensor sensitivity to hydrogen. The
SEM and TEM images of the composite are shown in Fig. 1: Pt is evenly
distributed on the surface of graphene, and no aggregation can be
observed. Despite a response of 15.1% for a hydrogen concentration of
1%, this value can be achieved while restoring the sensor to its original
state within 10 s. The measurement conditions for the sensing process
require a high temperature of 200 ◦ C, which restricts the sensor appli­
cation. Palladium has a good solubility for hydrogen. It can decompose
hydrogen into hydrogen atoms, which speeds up the transmission of
electrons to graphene [95]. Therefore, palladium is often used to
fabricate hydrogen gas sensors. J. L. Johnson et al. [95] substituted
palladium with doped graphene, and they reported experimental results
superior to those obtained by D. T. Phan et al. [94]. At room tempera­
ture, these sensors reach a 72% response within 8 s for a hydrogen
concentration of 0.2%, while returning to the original state after 35 s.
When the concentration of hydrogen is constant, a response value of
113% can be achieved after 3 s at 100 ◦ C, and the recovery time of the
device is 7 s, as shown in Fig. 2.
Both D. T. Phan et al. [96] and R. Kumar et al. [70] chose to modify
graphene with two metals. Discontinuous palladium nanoparticles are
excellent nanostructures to measure low concentrations of hydrogen,
Fig. 1. SEM images of synthesized Pt-3D graphene (a) without and (b) with Pt NPs. TEM images of Pt-3D graphene at (c) low magnification and (d) high magni­
fication. Reproduced from Ref. [94] with permission from Elsevier.
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despite the fact that their conductivity reduces due to such discontin­
uous structures [97]. The introduction of metal particles into the orig­
inal metal graphene composite sensor can significantly improve its
conductivity. The biggest advantage of the experiment performed by D.
T. Phan et al. [96] consisted in reducing the hysteresis of the gas mea­
surement after a single metal modification by doping the Pd-G com­
posite sensor with Ni. The original Pd-G sensor exhibited a hysteresis
phenomenon, which could be reduced due to the characteristics of
nickel. Owing to the addition of Ni, the hydrogen molecules are pre­
vented from penetrating deeply into the Pd lattice. This results in a
reduction of the hysteresis effect, thus improving the sensor stability
[98,99]. R. Kumar et al. [70] used two metals (Pd–Pt) to enhance the
hydrogen gas sensitivity. Both metals are good hydrogen sensing ma­
terials, which exhibit a good hydrogen absorption effect and form free
hydrides (PdHx, PtHx) [100]. The combination of these two metals in­
creases the surface area and the lattice shrinkage effect [101], which
further enhances the sensitivity of the sensors to hydrogen and improves
their response and recovery time. These experimental results show that
the maximum response value (5.1%) is achieved for a hydrogen con­
centration of 2% at a temperature slightly higher than room temperature
(40 ◦ C). Moreover, the response time is less than 2 s, and the recovery
time is 18 s.
3.2. Sensors for NH3 gas sensing
Ammonia is a reducing gas with a strong ability to supply electrons.
There are many oxygen-containing functional groups on the surface of
rGO. I. Karaduman et al. [69] doped graphene with silver, gold, and
platinum, and carried out a series of gas sensing experiments. Ag can
catalyze ammonia into active radicals and enhance the interaction be­
tween oxygen ions and ammonia molecules on the rGO surface [102].
The addition of Au and Pt improves the electronic transmission ability of
graphene, thus resulting in an enhancement of the sensitivity of
C. Wang et al.
Fig. 2. Sensing performance of the H2 sensor using Pt-3D graphene: (a) Influence of the working temperature, (b) transient response to various H2 concentrations, (c)
hysteresis, and (d) linearity properties. Reproduced from Ref. [94] with permission from Elsevier.
graphene-based sensors to several gases. Their experimental results
show that the three sensors have a good selectivity (Fig. 3), repeatability
(Fig. 4), and sensitivity to ammonia. Fig. 5 illustrates that the sensors
with the highest response measure changes of 1%, 0.25%, and 0.8%
when exposed to ammonia at a low concentration (0.1 ppm) at room
temperature. Moreover, their response and recovery time range between
a few seconds to a dozen seconds. The detection limits of these three
types of sensors were found to be 1.2, 16, and 1.6 ppb. This performance
is superior to that of many currently used ammonia sensors, and it is
likely that these sensors will have more important applications in the
future.
Fig. 3. Selectivity measurements of (a) AgNPs-rGO, (b) AuNPs-rGO, and (c)
PtNPs-rGO for NH3, H2, CO, and CO2 gases (1 ppm) at room temperature.
Reproduced from Ref. [69] with permission from Elsevier.
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3.3. Sensors for H2S gas sensing
O. Ovsianytskyi et al. [103] used a simple and clever method to dope
graphene with silver and iron ions in solution. Moreover, they success­
fully fabricated a sensor for hydrogen sulfide gas detection. The prop­
erties of such doped graphene-based gas sensors have been greatly
improved. Ag and Fe have a high affinity for H2S. In presence of Ag and
Fe, H2S dissociates and releases electrons. Since graphene is a p-type
semiconductor, the release of electrons reduces the number of holes and
leads to a change in conductivity. For this reason, this doping method
increases the sensing performance of the device. The experimental data
shows that, when testing in a low concentration of hydrogen sulfide gas,
the sensor response was close to 37%. Furthermore, it recovered in less
than six minutes and could be reused within a short time. At the same
time, the detection limit of this type of sensor was reduced to below
100 ppb, and the data shows that its sensitivity performance is excellent.
Since different metals have a different catalytic effect on different
gases, composite sensors consisting of graphene doped with a metal can
be used to sense a large variety of gases. For instance, Pt and Pd can
catalyze hydrogen, Ag can catalyze ammonia, and Fe and Ag can cata­
lyze H2S. When these devices are compared with a pure metal or pure
graphene sensor, the performance of the two-material sensor is signifi­
cantly higher. Moreover, this device exhibits a better selectivity. The
excellent catalytic effect of the metal on the gas, together with the large
specific surface area of graphene, enables the catalytic reaction to occur
and increases the excellent sensing performance of such device. In order
to detect different gases, it is necessary to find a metal with a high
catalytic effect on the target gas. With the aim of improving the sensor
characteristics, the shape and size of the metal nanocrystals can be
designed and improved [104], and the defect structures of the metal
surface can be modified to improve the catalytic activity of the metals.
This in turn improves the sensitivity of the sensors [105]. The
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Fig. 4. Repeatability for the (a) AgNPs-rGO, (b) AuNPs-rGO, and (c) PtNPs-rGO devices exposed to 0.1 ppm of NH3 gas. Reproduced from Ref. [69] with permission
from Elsevier.

Fig. 5. Sensing responses of (a) AgNPs-rGO, (b) AuNPs-rGO, and (c) PtNPs-rGO for different concentrations of NH3, H2, and CO gases at room temperature (Inset:
Calibration plots of NH3 for each proposed sensor). Reproduced from Ref. [69] with permission from Elsevier.

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functioning principle of this sensor is based on electron transfer between

the gas molecules and graphene. The optimization of the graphene
structure as well as the doping of several functional groups with a strong
adsorption capacity for a target gas results in an improvement of the
electron transfer rate and sensor conductivity, thereby enhancing its gas
sensitivity. GO/rGO-based gas sensors doped with metals have been
widely investigated. In this review, several results on these sensors are
reported in Table 1.

4. Graphene-based gas sensors doped with polymers

4.1. Sensors for NH3 gas sensing

X. L. Huang et al. [110] fabricated a gas sensor for ammonia detec­

tion using polyaniline and rGO. Their experimental results show that the
composite gas sensor is more sensitive and selective than a pure gra­
phene or polyaniline sensor. Indeed, its response to 50 ppm of ammonia
at room temperature is as high as 59.2%. The experimental data shows Fig. 6. Response curves of (a) the RGO-PANI hybrids, (b) bare PANI nanofibers,
that this value is significantly better than in the case of a pure graphene and (c) bare RGO to NH3 gas with a 50 ppm concentration. Reproduced from
(5.2%) and polyaniline (13.4%) gas sensor, as shown in Fig. 6. On the Ref. [110] with permission from the Royal Society of Chemistry.
one hand, PANI is an acid-base sensor with excellent performance,
which has good sensing characteristics for alkaline gases, such as
ammonia. On the other hand, graphene is a p-type semiconductor, and
ammonia has a strong electronic supply capacity: Once ammonia at­
taches to its surface, the number of holes is reduced and the resistivity
changes significantly. Moreover, as shown in Fig. 7, by comparing the
response of the sensor to different types of gases, such as methanol and
dichloromethane, it is found that the sensor response to ammonia gas is
much higher than for other gases: this result indicates that it has a good
selectivity for ammonia. One issue is represented by the fact that
ammonia is an alkaline gas, while polyaniline is an acidic substance.
Although polyaniline as a sensor exhibits a high response and selectivity
to ammonia, after being exposed to ammonia, it is difficult to recover its
initial state. The experimental results show that the resistance can be
restored to 80% of its original value, indicating that this kind of sensor
does not have a good repeatability, restricting its application in practice.
In order to solve this problem, decomposition agents can be added to
decompose the reaction products of polyaniline and ammonia after the
experiment.

4.2. Sensors for H2S gas sensing

S. Cho et al. [111] synthesized a graphene-based gas sensor doped Fig. 7. Response of the bare graphene device and of the RGO-PANI hybrid
with poly (4-styrenesulfonic acid)-doped (PSS-doped) polyaniline sensor to 20 ppm of NH3 and comparison with other analytes diluted to 1% of
the saturated vapor concentrations. Reproduced from Ref. [110] with permis­
hydrogen sulfide. Its possible sensing mechanism is shown in Fig. 8: H2S
sion from the Royal Society of Chemistry.
dissociates into H+ and HS− ions under the action of PANI. At this point,
PANI combines with H+. The doping with PSS induces the formation of
larger and smoother PANI particles, which increase the transport speed
of the carriers. In addition, the sulfonate anions (–SO−3 ) on PSS absorb

Table 1
Gas sensors based on graphene-metal nanohybrids.
Gas Material Working temperature (◦ C) Concentration Response Response/recovery time LOD ref

H2 Pt/G 200 10000 ppm 15.1% <10/<10 s – [94]

Pd/G 20 2000 ppm 72% ~8/35 s – [95]
Pd/G 100 2000 ppm 113% 3/7 s – [95]
Ni/Pd/G RT 1000 ppm 11% 3/12 min 1 ppm [96]
Pt/Pd/G – 2% 4% 2/60 s – [70]
Pt/rGO RT 1000 ppm 14% – – [106]
Pd/G RT 1000 ppm 33% 15/25 min 20 ppm [107]
Pd/G – 1% 50% 1/2 min – [108]
Pd/G 50 1000 ppm 7% 4/20 min 0.2 ppm [109]

NH3 Ag/rGO RT 0.1 ppm ~1% 5/6 s 1.2 ppb [69]

Au/rGO RT 0.1 ppm ~0.25% 13/17 s 16 ppb [69]
Pt/rGO RT 0.1 ppm ~0.8% 7/8 s 1.6 ppb [69]

H2S Ag/G RT 500 ppb 5% – 100 ppb [103]

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Fig. 8. Possible mechanism for the molecular interactions between the PSS-doped PANI/graphene nanocomposites and H2S gas molecules. Reproduced from
Ref. [111] with permission from the Royal Society of Chemistry.
the remaining H2S. Therefore, doping with PSS further increases the
conductivity of the sensor and H2S adsorption. The charge transfer is
mostly carried out via the graphene coordination. They fabricated a
series of sensors with different proportions of graphene and polyaniline
and found that graphene with a 30 wt% content exhibits the best char­
acteristics. Its response to 50 ppm of hydrogen sulfide at room temper­
ature is 78%, and it still maintains a significantly high response for a
concentration limit of 1 ppm. Furthermore, this type of sensor has a very
fast response (90 s) and recovery time (150 s), which are much faster
than other hydrogen sulfide-based sensors. Moreover, when exposed to
hydrogen sulfide for a long time, the sensor response value shows almost
no change, indicating that it can be reused several times. The results
show that it has a much higher response to hydrogen sulfide than
ammonia and ethanol, proving its good selectivity to hydrogen sulfide.
4.3. Sensors for CH4 gas sensing
Z. Q. Wu et al. [112] prepared a series of polyaniline/graphene
sensors with different mass ratios for methane detection. Compared with
pure polyaniline CH4 gas sensors, PANI-G gas sensors have a higher
sensitivity and wider measurement range owing to their larger specific
surface area. The response value for these sensors is ~3 in 100 ppm of
methane gas at room temperature, and the response and recovery times
are 85 and 45 s, respectively.
During the past several years, many studies have been conducted on
graphene-based gas sensors doped with a polymer. Here, several results
are listed in Table 2. Table 2 shows that almost all these sensors work at
room temperature and that their detection limit is extremely low.
However, when the polymer is compounded with graphene, it forms a
hybrid film [110] which, if too dense, prevents the gas molecules from
coming in contact with graphene. Therefore, in order to obtain excellent
Table 2
Gas sensors based on graphene-polymer nanohybrids.
gas Material Working temperature (◦ C) Concentration
NH3 PANI/rGO RT 50 ppm
PANI/G RT 100 ppm
G/PEDOT RT 500 ppm
PPy/rGO RT 3 ppm
H2S PANI/G – 50 ppm
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sensing results, the polymer hybrid film has to be manufactured into a
uniform film to allow for the contact with the gas molecules.
5. Graphene-based gas sensors doped with metal oxides
5.1. Sensors for NO2 gas sensing
Z. Y. Wang et al. [116] used an improved hydrothermal method to
obtain a highly sensitive graphene-based sensor doped with SnO2 for
nitrogen dioxide detection. The SEM and TEM images of the material
structures are shown in Figs. 9 and 10, respectively. These images show
a fold structure on the rough surface of the material and a uniform
distribution of small metal oxide particles on the surface. Their experi­
mental results show that the sensor can reach a response value of 227.6
in less than six minutes (405 s) when exposed to a concentration of
350 ppb of nitrogen dioxide gas at 75 ◦ C. Moreover, it can recover in
52 s, as shown in Fig. 11. When compared to a pure SnO2 sensor, the
response value is six times higher, and the response and recovery times
are both shorter. In addition, this sensor exhibits a detection limit of
50 ppb (Fig. 12). This indicates that the sensing performance of this type
of composite sensor is superior to that of other devices. When compared
to other gases, such as acetone and ethanol, the sensor response to NO2 is
200 times higher. Fig. 13 shows that this sensor has a good selectivity to
nitrogen dioxide. Fig. 14 illustrates the band model of SnO2/rGO, which
reveals the sensing mechanism for NO2. The potential barrier of the
heterojunction formed by the presence of the two semiconductors
changes due to the adsorption-desorption modulation of the gas mole­
cules, thus inducing a change in resistivity.
J. Liu et al. [117] reported a graphene NO2 sensor modified with
flower-like zinc oxide. The sensor shows an excellent sensitivity and a
high response at 100 ◦ C. The response value (S = 12) when exposed to
Reponse Reponse/recovery time LOD Ref.
59.2% 18/~2.4 min – [110]
~86.7% 50/23 s 1 ppm [113]
9.6% ~3/5 min <10 ppm [114]
1.105% 400/- s 3 ppm [115]
~78% 90/150 s 1 ppm [111]
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Fig. 9. FESEM images of (a, b) SnO2 and (c, d) SnO2/rGO. Reproduced from Ref. [116] with permission from Elsevier.

Fig. 10. (a, b) Typical TEM images and (c) HRTEM image of the SnO2/rGO composite. Reproduced from Ref. [116] with permission from Elsevier.

50 ppb of gas is seven times higher than that of a pure ZnO sensor under
the same conditions. Furthermore, it was found that the detection limit
is 5 ppb for a graphene concentration of 1.7 wt%. The response of the
sensor to NO2 is much higher than to other gases, indicating its high
selectivity. Fig. 15 shows that its original value can be recovered after
each detection, showing an excellent stability and repeatability. Y. Xia
et al. [118] reported a graphene-based gas sensor doped with ZnO. Their
experimental results show that this type of sensor has a higher response
to NO2 gas, a faster response and recovery time, a lower detection limit,
and a better selectivity, repeatability, and stability than other sensors.
J. Liu et al. [119] fabricated a sensor with a high response to NO2 by
modifying graphene with flower-like indium oxide. The experimental
data shows that a sensor with a 3 wt% concentration of graphene ex­
hibits the best performance. Its response value to 1 ppm of gas at 74 ◦ C is
1337: This value is seven times higher than that of a pure In2O3 sensor.
Its detection limit is 10 ppb, which is much lower than that of a pure
In2O3 gas sensor (40 ppb). These parameters are valid only for NO2 gas,
but not for other gases. Owing to the high specific surface area of the
flower-like indium oxide, the sensor is very sensitive to this gas. F. B. Gu
et al. [120] also performed similar experiments: Their results show that
the sensor has a high detection performance to NO2 gas. The sensor
response to NO2 is far higher than to other gases, indicating that it has a
good selectivity for NO2.
S. Srivastava et al. [121] prepared a NO2 sensor by modifying

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Fig. 11. Response of the sensors based on the SnO2/rGO composite and SnO2 to
350 ppb of NO2 as a function of the operating temperature. The insets show the
response transient curves of SnO2/rGO and SnO2 to 350 ppb of NO2 at 75 ◦ C and
65 ◦ C, respectively. Reproduced from Ref. [116] with permission from Elsevier.
Fig. 12. Response of the sensor based on SnO2/rGO to different concentrations
of NO2 at 75 ◦ C. Reproduced from Ref. [116] with permission from Elsevier.
Fig. 13. Response of the sensor based on the SnO2/rGO composite to various
gases at 75 ◦ C. Reproduced from Ref. [116] with permission from Elsevier.
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graphene with tungsten trioxide. When compared to pure graphene, to
pure WO3, and to a sensor consisting of 0.2 wt% and 0.5 wt% compos­
ites, the 0.5 wt% sensor performs best. Its response value to 5 ppm NO2
at 250 ◦ C is 133, and its detection limit is of only 1 ppm.
Several other researchers have performed investigations on metal
oxides-doped graphene-based NO2 gas sensors, some of which are
summarized in Table 3.
5.2. Sensors for ethanol gas sensing
C. H. Zhao et al. [151] fabricated a graphene-based sensor for the
detection of ethanol gas. The device was modified by adding SnO2
nanoparticles. Its performance was greatly improved with respect to a
pure graphene sensor. For a 100-ppm concentration of ethanol, this
composite sensor requires a lower temperature (250 ◦ C) to display a
higher response (S = 17.7).
S. M. Liang et al. [152] manufactured ZnO-doped graphene to detect
ethanol gas. Their experimental results show that the response (S = 513)
of this sensor is about four times higher than that of a pure ZnO sensor
for an ethanol gas concentration of 1000 ppm at 400 ◦ C. In addition,
they also tested its response to other gases, such as methanol and
acetone, and found that its response to ethanol is particularly high,
indicating that this sensor exhibits a good selectivity for ethanol gas.
M. H. Tian et al. [153] reported an ethanol gas sensor based on
Co3O4-doped graphene. They found that graphene with a 15 wt% Co3O4
concentration exhibits the best sensing properties. The response value of
this sensor when exposed to an ethanol gas concentration of 100 ppm at
200 ◦ C is 21, which is about three times as high as that of a pure Co3O4
ethanol sensor. Moreover, the sensor shows an excellent selectivity to
ethanol.
5.3. Sensors for NH3 gas sensing
Q. Q. Lin et al. [154] fabricated a flower-like SnO2 structure into
graphene to obtain a sensor to detect ammonia gas. This sensor consisted
of a three-dimensional (3D) structure, which was produced via the hy­
drothermal method. The biggest advantage of this sensor is its very fast
response time, lower than one minute in presence of a relatively lower
concentration of ammonia at room temperature. The effect of the hu­
midity has to be eliminated, since the water molecules can compete with
the target gas molecules, generating an impact on the resistance of the
sensor.
G. Singh et al. [155] reported a GO-based gas sensor doped with ZnO.
Their study shows that the device has a good response (24%) to very low
concentrations (1 ppm) of ammonia at room temperature. Moreover, its
original state can be restored in a few minutes. This indicates that this
method provides a support for the development of highly sensitive and
stable ammonia sensors in the future.
5.4. Sensors for acetone gas sensing
P. P. Wang et al. [156] reported a GO-based sensor doped with ZnO,
which was used for acetone detection. Similarly, L. L. Guo et al. [157]
used α-Fe2O3-doped rGO. J. N. Zhang et al. [158] reported that the
GO-based gas sensor doped with WO3 can be used for the detection of
acetone. Although they used different materials to dope graphene, the
experimental results point towards the same conclusion. These three
devices are able to detect 100 ppm of acetone gas with a very fast re­
covery speed, ranging from a few seconds to a dozen seconds. However,
the experimental results of L. L. Guo et al. [157] show that the response
value (S = 8.9) is much lower than that reported by P. P. Wang et al.
[156] (S = 35.8) and J. N. Zhang et al. [158] (S = 35.9). None of these
experiments was carried out at a high temperature (>200 ◦ C), and this
limits the development of practical applications for this type of sensors.
C. Wang et al.
Fig. 14. Schematic physical model and energy band model for the sensing mechanism of the NO2 sensor based on the SnO2/rGO composite in (a) air and (b) in NO2
atmosphere. Reproduced from Ref. [116] with permission from Elsevier.
Fig. 15. Reproducibility of the temporal response of the 1.7% rGO/ZnO hybrid
to 10 ppb of NO2 at 100 ◦ C. Reproduced from Ref. [117] with permission
from Elsevier.
5.5. Sensors for H2S gas sensing
J. J. Shi et al. [159] inserted WO3 into rGO and obtained a
three-dimensional structure for the detecting hydrogen sulfide gas. This
was a successful attempt since this sensor has a very low detection limit
for hydrogen sulfide and maintains a high response value (168.58) even
when the concentration reaches 40 ppm. The response value of the
sensor is about three times higher than that of a pure WO3 sensor under
the same conditions. These results were obtained for a graphene doping
concentration of 3.8 wt%. After a repeated comparison with other sen­
sors for the detection of other gases, it was found that the device shows a
good selectivity and stability for hydrogen sulfide gas. However, such
experiments were carried out at a high temperature (330 ◦ C). If a novel
method to obtain these results at room temperature was to be developed,
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this sensor would have almost no competitors in detecting hydrogen
sulfide gas. T. V. Cuong et al. [160] reported a sensor with a high
response to 2 ppm of hydrogen sulfide gas at room temperature. This
detector was fabricated with ZnO and graphene. However, since the air
is mainly composed of nitrogen, maintaining a high sensitivity for a long
time in a nitrogen environment is a limitation that still needs to be
addressed.
5.6. Sensors for SO2 gas sensing
P. Tyagi et al. [161] obtained a composite sensor using SnO2 and rGO
for detecting sulfur dioxide gas. Both materials exhibit a large specific
surface area, which has been used in the development of gas sensors for a
long time. The experimental results obtained with these devices are
impressive: Both a good response to SO2 at low concentrations and a
very fast response/recovery speed were obtained. Thus, this sulfur di­
oxide gas detection sensor is likely to find more applications in the
future.
5.7. Sensors for formaldehyde gas sensing
S. F. Shao et al. [162] fabricated a simple three-dimensional gas
sensor using TiO2 and graphene. The response value of this sensor can
reach 9.1 when the formaldehyde concentration is as low as 100 ppb,
and the response and recovery time are both only ~20 s. The only
drawback for this senor is that it needs to work at a high temperature of
150 ◦ C. In addition, X. F. Chu et al. [163] reported a sensor with good
response value (up to 3.9) at lower formaldehyde concentrations
(1 ppb). Additionally, both the response and recovery speed of this senor
are very fast, being 24 and 12 s, respectively. However, this sensor also
requires to work at a high temperature (133 ◦ C).
5.8. Sensors for CO2 gas sensing
M. Amarnath et al. [164] fabricated a carbon dioxide sensor via the
addition of indium into a NiO-rGO composite. The sensing electrode is
C. Wang et al. Ceramics International 47 (2021) 16367–16384

Table 3
NO2 sensors based on graphene-metal oxide nanohybrids.
Material Working temperature (◦ C) Concentration Reponse Reponse/recovery time LOD ref

SnO2/GO RT 5 ppm 1.203 40/357 s 450 ppb [122]

SnO2/CNTs/rGO RT 5 ppm 2.53 8/77 s – [123]
SnO2/rGO 50 5 ppm 3.31 135/200 s – [124]
SnO2/rGO RT 50 ppm ~6% 190/224 s – [125]
SnO2/rGO 150 5 ppm 26.342 13/- s 50 ppb [126]
SnO2/rGO RT 5 ppm 1.38 45/168 s – [127]
SnO2/RGO 45 100 ppm 1.08 -/373 s – [128]
SnO2/RGO 200 4 ppm 4.56 10/20 s 0.5 ppm [129]
SnO2/G RT 10 ppm 0.25 -/338 s – [130]
SnO2/RGO RT 5 ppm 1.203 40/357 s – [131]
SnO2/RGO 55 100 ppm 1.079 -/373 s – [132]
SnO2/G RT 50 ppm – 190/224 s – [133]
SnO2/rGO 60 1 ppm 12.7% − /− 15.7 ppb [134]
SnO2/rGO 200 10 ppm 247.8 39/15 s – [135]
SnO2/rGO RT 1 ppm 3.8 14/190 s 50 ppb [136]
SnO2/rGO 200 2 ppm 124 30/230 s 0.4 ppm [137]
ZnO/rGO 400 5 ppm ~125 143/259 s – [138]
ZnO/rGO RT 100 ppm 47.4% 6.2/15.5 min 5 ppm [139]
ZnO/rGO RT 5 ppm 25.6% 165/499 s – [140]
ZnO/rGO RT 50 ppm 9.61 25/15 s – [141]
ZnO/G RT 50 ppm 8% 132/164 s – [142]
ZnO/rGO RT 0.1 ppm 4.66 1.5/2.5 min 50 ppb [143]
WO3/rGO 250 5 ppm 133 − /− 1 ppm [121]
WO3/rGO 250 5 ppm 133 − /− – [144]
rGO/In2O3 74 1 ppm 1337 208/39 s 10 ppb [119]
In2O3/rGO RT 5 ppm 37.81% − /− – [145]
In2O3/rGO RT 30 ppm 8.25 4/24 min – [120]
Co3O4/rGO RT 60 ppm 5 600/- s – [146]
α-Fe2O3/rGO RT 90 ppm 150.63% -/1648 s – [147]
CuO/rGO RT 1 ppm 14 66/34 s – [148]
MoS2/G 200 10 ppm 69% 0.7/0.9 s 0.2 ppm [149]
TiO2/G RT 70–1775 ppb 1.17–3.14 35/90 s 50 ppb [150]

reduced as a consequence of the addition of indium, thus the perfor­
mance of the sensor is improved. The response of the sensor is 40%
under a CO2 concentration of 50 ppm at room temperature, and the
detection limit can reach 5 ppm. The response and recovery time for this
sensor are also very fast, being only 6 and 18 s, respectively.
5.9. Sensors for O3 gas sensing
WO3 is one of the materials with the highest response to ozone. Y. Liu
et al. [165] used WO3 and graphene as composite sensors to improve the
sensing performance to ozone. Compared with pure WO3, the working
temperature of the composite sensor can be reduced from 250 ◦ C to
150 ◦ C. In addition, in the presence of a low O3 concentration, the
response value can be as high as 380. Moreover, the response and

Table 4
Gas sensors based on graphene-metal oxide nanohybrids.
Gas Material Working temperature (◦ C) Concentration Reponse Reponse/recovery time ref

ethanol SnO2/G 250 100 ppm 17.7 9/457 s [151]

ZnO/G 400 1000 ppm 513 − /− [152]
α-Fe2O3/G 280 1000 ppm 30 − /− [167]
Co3O4/rGO 200 100 ppm ~21 − /− [153]

NH3 SnO2/GO RT 50 ppm 15.9% <1/<1 min [154]

Co3O4/rGO RT 50 ppm 53.6% − /− [168]
ZnO/rGO – 50 ppm 3.05 84/216 s [169]
ZnO/G RT 1 ppm ~24% ~6/~2–3 min [155]
ZnO/rGO 300 50 ppm 19.2% 50/250 s [170]

acetone TiO2/rGO 300 300 ppm 14 − /− [171]

ZnO/GO 240 100 ppm 35.8 13/7 s [156]
α-Fe2O3/rGO 375 100 ppm 8.9 3/9 s [157]
WO3/GO 375 100 ppm 35.9 4/10 s [158]

H2S MoO3/rGO 160 50 ppm 4120% − /− [172]

SO2 SnO2/rGO 60 500 ppm 22 2.4/3.5 min [161]

CO2 NiO/rGO – 500 ppm 83% 16/22 s [173]

HCHO SnO2/rGO 130 10 ppm 435 − /− [174]

SnO2/rGO 160 100 ppm 138 <20/<20 s [175]
SnO2/rGO 120 1 ppm 4.9 1/85 s [176]
ZnO/G 200 100 ppm 12 10/29 s [177]
SnO2/GO 120 100 ppm 32 66/10 s [178]

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recovery time for this sensor are very short, being only 17.1 and 32.7 s,
respectively.
5.10. Sensors for CH4 gas sensing
D. Z. Zhang et al. [166] reported a high-performance sensor
composed of NiO and rGO. The sensing performance is closely related to
the methane concentration and working temperature. In the work by D.
Z. Zhang et al., the response of the sensor was found to be 15.2% for
1000 ppm of CH4 at 260 ◦ C.
Several other studies on graphene-based gas sensors doped with
metal oxides have been performed to find approaches to enhance the
performance of various gas sensing techniques. The most relevant ones
are listed in Table 4. Tables 3 and 4 show that, although graphene
sensors with metal oxide composites can work at room temperature,
their responses are relatively low. Indeed, only at higher temperatures
they exhibit a very high response. The proportion of graphene in the
composite process significantly affects the gas sensing properties. If the
proportion of graphene is too large, the active sites are covered, limiting
the gas adsorption [117]. In order to further improve the sensing char­
acteristics of this sensor, its structure and doping ratio should be
investigated and optimized to define the extension of the specific surface
area and the active sites for gas sensing. Finally, in order to improve the
sensor selectivity to different gases, the Fermi energy level of the sensing
material should be controlled by adjusting the adsorption capacity of
oxygen to match the oxidation capacity of different gases [153].
results show that this type of sensor has a good selectivity and is likely to
be used for the detection of hydrogen in the future.
In the case of graphene-based sensors doped with metal-polymer
mixed materials, polymer/rGO behaves as a p-type semiconductor.
The carrier transport between the polymer/rGO material and the metal
particles constitutes the main sensing mechanism of such sensor.
Therefore, controlling the doping ratio of these three compounds rep­
resents the best method to achieve a high carrier transport efficiency. In
Section 3, it is mentioned that graphene-based sensors doped with
metals generally require a high temperature to provide optimal results.
However, due to the presence of the polymer, such sensors can also be
used at room temperature, overcoming the high-temperature limit
(Table 5). Moreover, the catalysis of the metal into the gas also mitigates
the decrease in gas sensitivity due to the dense structure of the polymer.
6.2. Graphene-based gas sensors doped with metal-metal oxide systems
Z. Y. Wang et al. [180] doped a SnO2-rGO sensor with Pd nano­
particles. Fig. 16 illustrates the two-step wet chemistry process that they
used. The most significant improvements obtained in the sensor per­
formance after doping consist in: (1) an extremely fast response to a low

6. Graphene-based gas sensors doped with two materials

6.1. Graphene-based gas sensors doped with a metal-polymer systems

Several metals exhibit a good response to specific gases. For this

reason, it would be beneficial to enhance the composition of graphene-
based sensors with polyaniline and metals. Palladium, for example, has a
good response to hydrogen. Y. J. Zou et al. [179] made the first attempt
to synthesize a palladium-doped rGO/polyaniline composite hydrogen
sensor. The excellent catalytic effect of palladium on hydrogen together
with the large specific surface area of PANI/rGO provides suitable re­
action sites, which improve the device sensing capability for hydrogen.
Their experimental results show that the sensor has linear characteristics
for different concentrations of hydrogen. Furthermore, for a limit con­
centration of 0.01 vol%, the sensor still shows a response of ~5% and
only a few tens of seconds for the response/recovery time. When
Fig. 16. Schematic illustration of the synthesis of the Pd–SnO2-RGO hybrids.
compared to other sensors, its response to hydrogen is especially high,
Reproduced from Ref. [180] with permission from Elsevier.
reaching a ten-time larger threshold than that to other gases. These

Table 5
Graphene-based sensors doped with two nanohybrids.
Material Gas Working temperature (◦ C) Concentration Response Response/recovery time Ref.

Pd/PANI/rGO H2 RT 1 vol% 25% 20/50 s [179]

Pd/SnO2/rGO NH3 RT 5 ppm 7.6% 7/50 min [182]
Pd/SnO2/G H2 200 2000 ppm 14.8% 34/27 s [183]
Pd/WO3/rGO H2 100 100 ppm 72 35/37 s [184]
Au/ZnO/rGO CO 400 5 ppm 35.8 177.3/76.1 s [185]
Nb/TiO2/rGO CO 380 800 ppm 6.2 − /− [189]
Au/SnO2/rGO NO2 50 5 ppm 1.6 19/20 s [190]
In/SnO2/rGO NO2 – 100 ppm 11 400/~ s [191]
Ag/SnO2/rGO NO2 – 1 ppm 3.92 13/105 s [192]
Fe/WO3/rGO NO2 RT 3 ppm 5.9% 6.7/5.4 min [193]
Pd/SnO2/rGO NH3 RT 5 ppm 7.6% 7/50 min [182]
Gd/WO3/rGO acetone 200 50 ppm 55 − /− [194]
Pd/SnO2/G H2 200 2000 ppm 14.8% 34/27 s [183]
PANI/SnO2/rGO NH3 RT 20 ppm 160% 11/28 min [186]
PPy/TiO2/G NH3 RT 50 ppm 102.2% 36/16 s [187]
PANI/ZnO/G acetone RT 2 ppm 11.56% 15/27 s [188]
PANI/ZnO/G acetone RT 5 ppm 25.6% 22/30 s [188]
PANI/SnO2/rGO H2S RT 200 ppb 23.9 − /− [195]

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concentration of NO2 gas at room temperature, and (2) a stable detec­

tion limit. The incorporation of the Pd nanoparticles promotes the
decomposition and adsorption of O2 onto the SnO2 surface, thus
significantly enhancing the electron transfer. In addition, the nano­
particles provide activation sites for the adsorption of NO2, thus
enhancing the sensor response [181].
P. G. Su et al. [182] introduced palladium and tin oxide into rGO to
obtain a composite sensor. Owing to the presence of palladium atoms
onto the SnO2-rGO surface, both the adsorption and reduction of the
ammonia gas concentration were significantly enhanced. The results
show that the sensor fabricated using this method exhibits a higher
sensitivity to ammonia gas and can be used stably for two months.
S. Dhall et al. [183] introduced Pd into a SnO2-graphene gas sensor to
increase its detection limit for hydrogen. Palladium itself can be used as
a sensor to detect hydrogen owing to its high catalytic effect on
hydrogen, but its sensing performance can be further improved when it
is introduced into a SnO2/G structure. This device shows a rapid
response, an excellent recovery, and reusability. Similarly, A. Esfandiar
Fig. 17. Gas responses of the GN, PPy-GN, and TiO2@PPy-GN thin films to
et al. [184] introduced Pd into a sensor composed of tungsten trioxide
50 ppm of NH3 at room temperature. Reproduced from Ref. [187] with
and rGO, further improving its hydrogen sensing performance. Its
permission from Elsevier.
response value reaches 72 for a hydrogen concentration of 100 ppm, and
the response and recovery times are both ~30 s. Its selectivity for
hydrogen is excellent when compared to methane, carbon monoxide,
and other gases. Therefore, the introduction of Pd in metal oxides and
graphene composite sensors is beneficial to detect hydrogen.
Au is a good CO catalyst. Z. U. Abiden et al. [185] reported a carbon
monoxide sensor modified with gold, which is composed of zinc oxide
and rGO. This device has a very high sensitivity and a response value of
35.8 for a CO concentration of 5 ppm. However, such a sensitive
detection is possible only at a temperature of 400 ◦ C. Nonetheless, these
results are superior to those obtained with a pure ZnO sensor or a
ZnO-rGO sensor.
The metal oxide is the main electron provider in graphene-based
sensors doped with metal-metal oxide systems. For this reason, elec­
tron transfer from the metal oxide represents the main sensing mecha­
nism of the device. However, the presence of metal particles affects the
electron transfer, and controlling the metal doping amount is of pivotal
importance to improve the sensing capabilities. Although the working
temperature of such sensors is still high, their response is greatly
improved due to the catalytic effect of the metal on the gas.
Fig. 18. Gas response of the TiO2@PPy-GN-based sensor to 50 ppm of NH3 for
four adsorption and desorption cycles. Reproduced from Ref. [187] with
6.3. Graphene-based gas sensors doped with polymer-metal oxide systems permission from Elsevier.

In addition, several attempts have been made at incorporating metal

stable and has a good selectivity, as shown in Fig. 18. This indicates that
oxides onto the surface of graphene-based gas sensors, using a polymer
this sensor has a potential to be used in several applications in the future.
to further improve the sensitivity of the sensor to the gas. For example,
However, since the TiO2 properties are greatly affected by temperature,
Z. B. Ye et al. [186] reported a gas sensor based on a composite of rGO
these compounds cannot be used at a higher temperature, limiting the
and polyaniline doped with tin oxide. Tin oxide provides a matrix with a
working temperature range of the sensor.
high conductivity to foster the growth of PANI and inhibits its further
D. Z. Zhang et al. [188] developed a zinc oxide
polymerization. Their experimental results show that the response of the
graphene/polyaniline-based composite sensor for the detection of
sensor to the gas greatly improves (more than 100%); however the
acetone gas at the ppb-level. The addition of ZnO causes a larger number
response and recovery time do not seem to change significantly. This
of oxygen molecules to bind to the surface, thus providing sites for the
problem remains unresolved. However, the composite sensor of the
reaction with acetone. ZnO is a n-type semiconductor and PANI is a
graphene-based compound modified with polypyrrole and titanium di­
p-type semiconductor, thus their combination forms a heterojunction,
oxide reported by C. L. Xiang et al. [187] exhibits great advantages
further improving the sensing performance for acetone gas. A high
during the sensing tests of ammonia gas. Since titanium dioxide itself is a
response, low detection limit, good stability, and fast response/recovery
good sensing material used to detect ammonia gas and other gases, the
speed are the biggest advantages of this sensor, as shown in Fig. 19. Its
properties of the composite sensor can be improved with doping. At
response is higher than 90% for 50 ppm of acetone. If the concentration
room temperature, the response to 50 ppm of ammonia reaches 102.2%,
of acetone is decreased to its standard lower limit (500 ppb), the sensor
and the response and recovery speeds are very fast, being only 10–12 s
response remains close to 2%. When measured intermittently for a
(Fig. 17). When compared to gas sensors based on graphene or doped
month, the response maintains the same value. Furthermore, its
with polypyrrole, the performance of such sensor is higher. Moreover, its
response/recovery time is extremely short, being 15 and 27 s for 2 ppm
sensing limit is reduced to 1 ppm. TiO2 is a n-type semiconductor, and
of acetone and 22 and 30 s for 5 ppm of acetone.
the improvement of its properties may be due to the formation of p-n
In the case of graphene-based sensors mixed with polymer-metal
junctions between TiO2 and PPy-rGO. After several tests and compari­
oxide systems, polymer/rGO behaves as a p-type semiconductor,
sons with other gas sensors, the results show that this sensor is extremely

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Fig. 19. (a) Long-term stability of ZnO/S, N: GQDs/PANI film sensor with 2, 5,
and 20 ppm of acetone. (b) Response of the ZnO/S, N:GQDs/PANI film sensor as
a function of the relative humidity. (c) Gas sensing response of the ZnO/S, N
GQDs/PANI film sensor in the presence of 1 ppm of acetone after several
bending cycles. Reproduced from Ref. [188] with permission from Elsevier.
whereas the metal oxide is a n-type semiconductor and provides elec­
trons. Therefore, the main sensing mechanism of such sensor consists of
the electronic transmission between polymer/rGO and the metal oxide.
Controlling the ratio of the two semiconductor materials is key to obtain
an optimal sensing effect. Graphene-based devices doped with metal-
oxide composites need a high temperature to achieve good results. In
this case, the presence of the polymer mitigates the disadvantages
introduced by temperature and allows the sensor to work also at room
temperature (Table 5). Furthermore, the addition of the metal oxides
strengthens the n-type semiconductor behavior and introduces more
electrons. This improves the p-n junction between the metal oxide and
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Ceramics International 47 (2021) 16367–16384
polymer/rGO, enhancing the overall conductivity of the sensor and its
sensitivity to the gas.
To sum up, such sensor retains the advantages introduced by all its
components and overcomes several of their drawbacks. However, the
ratio of the different materials has to be carefully controlled in
graphene-based sensors doped with two mixed materials since their
working mechanism relies on the carrier transmission between the
materials themselves. Their amount directly affects the transmission
efficiency of the carriers, thus affecting the sensor sensing capabilities.
7. Conclusions and perspective
In this review, the latest research progress on graphene-based gas
sensors modified with the addition of metals, polymers, and metal ox­
ides is reviewed. These sensors exhibit a high response to gas and have a
good sensitivity, selectivity, repeatability, and stability. Several of the
review sensors can even work at room temperature. Moreover, their
response and recovery speed has been greatly accelerated. Therefore,
they are expected to play a pivotal role in several applications in the
future. However, these research results are still in the stage of laboratory
research; several investigations are needed to bring these results to an
industrial scale. However, most studies show that although the detection
limit can reach the ppb level, the response is not very high. Therefore,
research on the development of a highly-sensitive sensor must remain
the main goal.
Further investigations are needed to tackle a few open issues to
develop sensors with a higher sensitivity. (1) The air humidity has a
great influence on the sensor [154]; this means that the device can only
work in a relatively dry environment. (2) In some cases, the gas mole­
cules penetrate inside the metal lattice and induce a hysteresis phe­
nomenon. (3) The polymer-composite sensors do not show a long-term
stability. (4) The room-temperature response of the metal-oxide com­
posites is not ideal. These compounds need high temperatures to achieve
good sensing performance. For this reason, the working temperature
range of these devices is limited. (5) Doped nanoparticles constitute the
main electron source, and the ratio of dopants to graphene should be
carefully controlled during the production process. (6) The
three-dimensional structure of graphene is very fragile. For this reason,
the development of a new solid three-dimensional graphene framework
would be beneficial.
In the future, the following points have to be addressed when
choosing composite materials for graphene-based gas sensors. A good
moisture resistance, wide operating temperature range, large specific
surface area, suitable energy band difference, strong absorption-
desorption gas capacity, stable chemical properties, and good conduc­
tivity are all necessary features to develop sensitive devices. Based on
the available experimental results, the possible directions to improve the
sensing characteristics of such gas sensors are the following. (1) Opti­
mizing the structure of composite sensors and mixture doping ratio to
obtain a larger specific surface area. Moreover, increasing the number of
active sites is necessary to improve the sensor sensitivity. (2) Finding
catalysts with a higher catalytic effect and conductivity for chemical
doping to improve the response value of the sensor. (3) Incorporating
functional materials with a molecular screening function into the sen­
sors may improve their gas selectivity [196].
At present, there are many types of gas sensors on the market. For
example, a type of CO gas sensor called ES4-CO-100000 ppm is devel­
oped by EC Sense company in Germany. They apply solid polymer
electrochemical detection technology to fabricate this type of sensor.
The sensor is composed of three different metal electrodes as well as
electrolyte. Gas can diffuse into the working electrode of the sensor
when the electrode and electrolyte are exposed to air. Then the gas is
oxidized or reduced to produce a weak current signal. The weak signal is
collected by external electricity circuit and it’s converted into standard
signal output. The measurement limit of the sensor is 10 ppm and the
response time is about one minute. If we try to fabricate graphene-metal
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composite sensor, we may get lower measurement limit and faster
response speed. Another type of gas sensor called SGP gas sensor which
is developed by Sensirion company in Switzerland. SGP sensor is a
typical metal oxide gas sensor, which has a heating film inside. When the
sensor works, the heating film provides appropriate temperature con­
ditions to make the oxygen adsorbed on the metal oxide particles and
react with target gases, thus releasing electrons to change its resistance.
The disadvantage of this type of sensor is that it needs high working
temperatures. If we fabricate graphene-metal oxide composite sensor, its
working temperature can largely lower even to room temperature.
Declaration of competing interest
The authors declare that they have no known competing financial
interests or personal relationships that could have appeared to influence
the work reported in this paper.
Acknowledgments
The authors gratefully acknowledge financial supports by the Na­
tional Natural Science Foundation of China (no. 61871281 and
51302179), and the Priority Academic Program Development (PAPD) of
Jiangsu Higher Education Institutions.
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