1-s2.0-S135983682200751X-main

Composites Part B 248 (2023) 110378
Contents lists available at ScienceDirect
Composites Part B
journal homepage: www.elsevier.com/locate/compositesb
An overview on room-temperature chemiresistor gas sensors based on 2D

materials: Research status and challenge
Ziying Wang a, b, *, Miaomiao Bu b, Ning Hu a, b, **, Libin Zhao a, b, ***
a
State Key Laboratory of Reliability and Intelligence Electrical Equipment, Hebei University of Technology, Tianjin, 300130, PR China
b
School of Mechanical Engineering, National Engineering Research Center for Technological Innovation Method and Tool, School of Electronics and Information
Engineering, Hebei University of Technology, Tianjin, 300401, PR China
A R T I C L E I N F O A B S T R A C T
Keywords: It is necessary to develop efficient sensing materials, high-performance sensors and detailed mechanism study of
Two-dimensional materials (2DMs) chemiresistor gas sensors for applications in the fields of toxic gas monitoring, smart home, non-traumatic
Room-temperature (RT) disease marker, wearable electronics, etc. Two-dimensional materials (2DMs), including graphene, transition
Gas sensors
metal dichalcogenides (TMDs), black phosphorus (BP), graphitic carbon nitride (g-C3N4), MXenes, metal-organic
Flexible and wearable devices
Self-power and wireless technology
frameworks (MOFs), boron nitride (BN) and others, have proven to be attractive for fabrication of chemiresistor
gas sensors due to their unique structure and remarkable characteristics. A major focus of this paper on advances
and challenges in gas sensors based on 2DMs. Firstly, the electronic structure, physical and chemical properties
and semiconductor properties of 2DMs are described. Secondly, the synthesis methods and gas-sensitive prop
erties of 2DMs based gas sensors are introduced. In addition, strategies of improving gas sensors based on 2DMs
are also discussed. Finally, the developments trend for 2DMs based gas sensors is presented from the following
aspects: regulation of microstructure, contact between 2DMs and substrates, microelectromechanical systems
(MEMS) based gas sensors and gas sensor arrays, flexible and wearable gas sensors, smart self-power and wireless
gas sensors, theoretical calculation and in-situ characterization, influence of humidity on gas sensitivity.
1. Introduction semiconductor, electrochemical, solid electrolyte and contact combus

tion, etc.
In recent years, the requirements of gas sensors are dramatically
increasing in many different fields, such as air pollution monitoring in 1.1. Overview of semiconductor resistive gas sensors
atmospheric and indoor environment, military and aerospace security,
the detection of human health and food safety, etc. [1]. Gas sensors are The sensing materials are the key component of gas sensors, which
one of electrical transducers, which can sense the presence of toxic gases could interact with target gases. The design and preparation of sensitive
and quantify concentration of gases [2]. Gas sensors detect diverse materials with excellent properties is an effective way to improve gas
gases, including volatile organic compounds (VOCs, e.g., C2H5OH, sensing performance. In order to choose excellent gas sensing materials,
CH3COCH3, HCHO, C7H8, etc.), irritating gases (NH3, NOx, SO2, Cl2, some properties of the materials (e.g., surface microstructure, lattice
etc.) and asphyxiating gases (CH4, CH3CH3, CO, H2S, etc.). According to structure, electronic properties, semiconductor properties, flexibility as
the change of physical parameters (heat, light, sound, quality, etc.) and well as compatibility with substrates) should be considered. Generally,
the occurrence of chemical effects (chemical adsorption and redox re metal oxides are one of outstanding sensing materials, which are used to
actions, etc.), gas sensors are divided into physical and chemical gas fabricate resistive-type semiconductor gas sensors. Metal oxide-based
sensors. The type of physical gas sensors includes thermal conductivity, gas sensors have been extensively studied in the past several decades
optical, surface acoustic wave (SAW) and quartz crystal microbalance because of the merits of low cost, high sensitivities and easy fabrication
(QCM), etc. Besides, common chemical gas sensors are based on method [3].
* Corresponding author. State Key Laboratory of Reliability and Intelligence Electrical Equipment, Hebei University of Technology, Tianjin, 300130, PR China.
** Corresponding author. State Key Laboratory of Reliability and Intelligence Electrical Equipment, Hebei University of Technology, Tianjin, 300130, PR China.
*** Corresponding author. State Key Laboratory of Reliability and Intelligence Electrical Equipment, Hebei University of Technology, Tianjin, 300130, PR China.
E-mail addresses: wangzy@hebut.edu.cn (Z. Wang), ninghu@hebut.edu.cn (N. Hu), lbzhao@buaa.edu.cn (L. Zhao).
https://doi.org/10.1016/j.compositesb.2022.110378
Received 20 July 2022; Received in revised form 24 September 2022; Accepted 23 October 2022
Available online 29 October 2022
1359-8368/© 2022 Elsevier Ltd. All rights reserved.
Z. Wang et al. Composites Part B 248 (2023) 110378
1.1.1. The sensing mechanism of semiconductor resistive gas sensors

The sensing mechanism of metal oxide-based gas sensors can be
manifested by the model of chemisorbed oxygen. The change in the
resistance of metal oxide is affected by the surface reaction. The gas
chemisorption is an energy activated processes and oxygen species re
quires different temperature to take place on the grains surface. In air,
oxygen molecules capture electrons from materials and then exist as O−2
(<100 ◦ C), O− (100–300 ◦ C) and O2− (>300 ◦ C) on surface of materials
[4]. In general, relatively high temperature may endow adsorbed gas
molecules with high activation and could speed up the rate of gas
diffusion. It is conducive to the occurrence of chemical reactions be
tween oxygen species and target gas. The electron depletion layer is
formed on surface of n-type semiconductor and the hole accumulation
layer is formed on surface of p-type semiconductor. The resistance of
n-type metal oxides in air is high because of the potential barrier at grain
boundary [5]. When sensor is exposed to reducing gases, adsorbed ox
ygen reacts with reducing gases. Meanwhile, electrons captured by
adsorbed oxygen are returned to the surface of materials. Then, the
potential barrier and resistance of n-type metal oxides will decrease. The
resistance is changed in this process in order to realize the detection of
target gas.
1.1.2. The challenge of semiconductor resistive gas sensors

Although metal oxide gas sensors have many advantages, they need
to work at high temperature (150–300 ◦ C). The high temperature
environment induces the thermal growth of grains. At the same time, the Fig. 1. Schematics illustrating of room-temperature chemiresistor gas sensors
sensitivity, long-term stability and lifetime of the sensors will decrease based on 2D materials.
[6]. Several techniques have been widely adopted in preparing thick
sensitive films of metal oxide-based gas sensors, such as screen-printing s− 1) and high carrier density (1012 cm− 2) at RT [19]. The theoretical
of metal oxide powders, spin coating techniques, spray pyrolysis and so value of specific surface area is 2630 m2 g− 1 [20]. The bandgap of
on [7]. However, these preparation technologies of thick films and high monolayer graphene is zero, but bandgap and conductivity are accord
energy consumption of metal oxide gas sensors bring multiple chal ing to the number of layers.
lenges to the development of smart wearable devices. In addition to, the Graphene is used for applications in RT gas sensing due to its high
resistance of metal oxide gas sensors is very high, but sensitivity is low at conductivity, large specific surface area and low noise. Its 2D lamellar
RT. Although metal oxide gas sensors have been researched for decades, structure is favorable for the interaction between gas and graphene.
the development of gas sensors with low concentration, fast response After gas molecules are adsorbed on the surface, concentration of car
and recovery, high sensitivity as well as operating at RT present riers in graphene will change, which lead to the change of resistance.
challenges. Graphene can even detect individual gas molecule [21]. Besides,
outstanding mechanical and flexible performance of graphene are
1.2. Advantages of 2DMs for gas sensing compatible with flexible and wearable electronic devices [22].
In general, GO is prepared via classical and other modified Hum
2DMs belong to two-dimensional atomic crystal, whose thickness mer’s methods under strong acidic oxidation conditions [23]. Rich ox
could change from a few to tens of nanometers and size comes up to ygen containing functional groups (OCFGs) are retained on surface of
centimeter [8]. In 2004, Geim and Novoselov et al. firstly prepared GO. Meanwhile, compared to graphene, the conductivity of GO is
single and few-layer graphene via mechanical exfoliation (ME) suc decreased severely. In order to regain excellent conductivity, RGO can
cessfully [9]. The researchers of various scientific field have paid a lot of be obtained by thermal, light and chemical reduction treatments [18]. In
attention to graphene because of its remarkable mechanical, thermal, contrast to GO, the amount of C–O bonds of RGO is dramatically
optical, electrical and other properties [10]. Subsequently, other 2DMs decreased.
such as TMDs [11], BP [12], g-C3N4 [13], MXenes [14] and 2D Compared with pure graphene, RGO has more advantages as one of
conductive MOFs [15], etc. have also shown promising applications in carbon-based gas sensing material, which are mainly reflected in the
batteries, supercapacitors, solar cells, chemical and biological sensors, following aspects:
etc [16]. Several 2DMs can be used to fabricate chemical sensors
because of their remarkable physical and chemical properties (Fig. 1). In (1) As p-type semiconductor, charge transfer is happened between
general, several important parameters of gas sensors are used to char RGO and adsorbed gas molecules. The contact mode between
acterize gas sensing performance, such as response (or sensitivity), RGO and gas is changed from van der Waals force to a strong
selectivity, response and recovery times, and stability. covalent bond [24].
(2) The presence of defects, sp2 hybridized carbon atoms and OCFGs
1.2.1. The properties and advantages of graphene, GO and RGO for gas (e.g., epoxy, hydroxyl and carboxyl) in RGO can be used as active
sensing sites for gas adsorption [25].
The 2D bulk crystals are formed through van der Waals interaction of (3) The functional modification on the surface of RGO is easy to
layers. The atoms in the layers are connected to each other by chemical operate because of its lamellar structure and OCFGs, so as to
bonds [10]. In the hexagonal honeycomb lattice structure of graphene, regulate gas sensitivity [26].
each carbon atom is connected to three neighboring carbon atoms by a
σ-bond [17]. The distance between two carbon atoms is 1.42 Å in the 1.2.2. The properties and advantages of TMDs for gas sensing
same layer and the distance between neighboring layers is 3.35 Å [18]. 2D TMDs are MX2-type inorganic compounds, where M is the tran
Graphene displays an extremely high carrier mobility (2 × 105 cm2 V− 1 sition metal in IV, V, VI groups (Mo, W, Tc, Re etc.) and X is the
2
chalcogen (S, Se, Te etc.). The thickness of monolayer layered TMDs is and low resistivity [10,47].
~6–7 Å and the length of metallic bond is ~3–4 Å [27]. The band gap of As shown in Table 1, these 2DMs have their intrinsic unique crystal
monolayered TMDs can be changed between 1.0 and 2.2 eV, such as structure. The regulation of structure can change the bandgap and
MoS2 (1.8 eV), MoSe2 (1.5 eV), MoTe2 (1.1 eV) and WS2 (2.1 eV), which conductivity of 2DMs by the introduction of defects, the modification of
is tuned by controlled the number of layers of TMDs [28]. Besides, due to heterogeneous atoms and turning the number of layers and so on [39,
the absence of dangling bonds in TMDs, electron mobility of TMDs de 48]. Compared with bulks and other dimensions materials (0D, 1D and
vice is high when TMDs are deposited on appropriate substrates. For 3D), the most 2DMs possess larger surface-to-volume ratio, which is
example, the mobility of MoS2 is ~700 cm− 1V− 1s− 1 on SiO2/Si substrate beneficial for the interaction of gas and materials and further improving
[29]. The unique properties of MoS2, including lamellar structure, the chemical reactivity [39]. The change in conductivity of 2DMs is from
layer-dependent band gap and high electron mobility, which can insulator to the metal according to the difference of bandgap.
contribute to excellent RT gas sensing performance. Besides, charge In addition, the mechanism of gas sensors is associated with the
transfer mechanism is used to explain gas sensing process on the surface adsorption and reactions between gas molecules and materials. In gen
of TMDs [30]. The charge transfer process has been proved by density eral, there are two types of interactions between gas molecules and
functional theory (DFT) [31] and in-situ photoluminescence (PL) char materials: the non-covalent bonding interactions (VDWFs, π-π in
acterization [32]. Cho et al. have reported that negative adsorption teractions, and H-bond), covalent bonding interactions arising from the
energies (Eadv) were produced when NO2 and NH3 molecules were reaction and the charge transfer. When gases are adsorbed on different
adsorbed on MoS2 because of exothermic reactions. Meanwhile, the materials, different interactions are occurring (Table 1). The selection of
electron region of MoS2 by NO2 adsorbing leads to an increase in the interaction is determined by the structure of gases and materials.
intensity of the positively charged trions (A+) and a suppression of the Finally, they demonstrate good compatibility with the substrate due to
intensity of neutral excitons (A0), but electron accumulation by NH3 their atomic-size thickness and excellent flexibility. Therefore, 2DMs are
adsorbing is opposite process [32]. promising candidates for fabricating sensors owing to all of their
remarkable features.
1.2.3. The properties and advantages of other 2DMs for gas sensing
BP is another typical 2D crystal materials with unique layered 2. Applications of 2DMs in RT gas sensors
structure. Its structure is similar to that of graphene. The sp3 hybridized
P atoms construct a layered orthorhombic crystal structure [33]. Band 2.1. Graphene-based gas sensors
gap of BP is between 0.3 and 2.0 eV [34]. The band gap of BP thin film
(thickness of more than 4 nm) is ~0.3 eV [35] and band gap of BP with 2.1.1. Preparation of graphene
single molecular layer is ~2.0 eV [36], which demonstrates that band Graphene can be prepared by different methods, of which the four
gap is related to the number of BP layers. As a p-type material, BP is used main methods are as follows: mechanical exfoliation (ME) [9,49],
for applications in gas sensing resulting from its large specific surface chemical vapor deposition (CVD) [49–51], epitaxial growth [52] and
area, high carrier mobility (1000 cm2V− 1s− 1) at RT and tunable band chemical oxidation exfoliation [53]. The advantages and disadvantages
gap [37]. In addition, the wrinkled structure of 2D BP offers many active of these preparation methods for graphene are listed in Table 2.
sites for gas adsorption. Compared to other 2DMs (e.g., graphene, MoS2
and other TMDs), BP has higher adsorption energy for NO2 molecules (1) ME method
and lower out-of-plane conductivity. These properties contribute to the
enhanced gas sensitive performance [38]. Novoselov and Geim have used micro-mechanical exfoliation (M-
The g-C3N4 is also a typical layered semiconductor, which exhibits ME) method to delaminate highly ordered pyrolytic graphite (HOPG) as
2D conjugated s-triazine rings structure. The crystal structure of g-C3N4 early as 2004 to obtain single-layer graphene [9], and won the Nobel
is identified as N-substituted graphite framework, which is formed by Prize in Physics for their pioneering research results. Then, Coleman’s
sp2 hybridization of C and N. The band gap is adjustable in the range of research team used ultrasonic liquid phase stripping to prepare
~2.5–2.8 eV [39]. Except for the superior properties of g-C3N4 (e.g., high-quality graphene [49]. When graphite powder is dispersed with
large surface area, high conductivity and excellent thermal stability), different solvents (such as N-methylpyrrolidone (NMP), N, N-dimethy
the van der Waals forces (VDWFs) make g-C3N4 show a strong affinity for lacetamide (DMA), 1, 3-dimethyl-2-imidazolidinone (DMEU) and water,
gas molecules, which exist between layers and the chemical bonding of etc.), better dispersion effect can be obtained, especially DMA. Ultra
s-triazine units in each layer [40]. sonic treatment, delamination and exfoliation are used to prepare
Another potential 2D material is MXenes. MXenes are associated single-layer and multi-layer graphene.
with transition metal carbides, nitrides and carbonitrides, which are
obtained by etching of A element from MAX phases [41]. MAX phases (2) CVD method
have a layered and hexagonal structure with P63/mmc symmetry, where
M is transition metal (Ti, Cr, Nb, etc.), A is the element in IIIA or IVA After CH4 or C2H2 is introduced to the surface of the high-
group (Al, Si, In, etc.), and X (C or N) [42]. MXenes are suitable for RT temperature heated metal substrate for a period of time, the carbon
gas sensing applications leading cause of their high electrical and ther source decomposes on the metal substrate and graphene with different
mal conductivity, tunable electronic and chemical properties [43]. layers is deposited on the substrate, and then it is separated by chemical
MOFs are controllable porous nanostructured materials, which corrosion method [49–51].
consist of metal ions and organic ligands. The striking features (e.g.,
ultrahigh porosity, large surface area and facile structural adjustability) (3) Epitaxial growth method
make MOFs suitable for the application of supercapacitors, catalysts and
chemical sensors [44,45]. For gas sensing application, the special porous Graphene based on SiC surface was prepared by sublimation and
framework structure of MOFs not only can favor the interaction between reconstruction of Si atom under high temperature and high vacuum. The
gas and materials, but also facilitate surface reaction. Besides, as tem number of layers of graphene is determined by heat treatment time and
plates, MOFs are used to prepare porous metals and metal oxides, which temperature. Berger et al. obtained graphite thin films as large as the
have controlled morphologies, amounts of reaction sites and gas original single crystals by high temperature heating SiC single crystals in
permeability [46]. However, in contrast with three-dimensional (3D) 2004 [52].
MOFs, 2D conductive MOFs have received a lot of attention for gas
sensor application resulting from the wide range of high carrier mobility (4) Chemical oxidation exfoliation method
3
Table 1
The characteristic parameters of 2D materials for improving gas sensing at room temperature.
Materials Crystal structure Specific surface area (m2 Carrier mobility (cm2 V− 1
Bandgap Interaction between gas and materials
g− 1) s− 1) (eV)
Hexagonal 2630 [24] 2 × 105 [23] 0 π-π interaction and van der Waals [60,
61]
Graphene
2H, 1T, 1T′ , and 3R – ~700 [34] 1.0–2.2 [33] charge transfer [39]
TMDs (MoS2)
Orthorhombic C ~2630 [41] 600-1000 [45] 0.3–2.0 [42] charge transfer [62]
BP
triazine and tris-triazine/ 2500 [47] ~100 [48] 2.5–2.8 [49] π-π interaction, van der Waals [8]
heptazine
g-C3N4
Hexagonal – ~34 [53] 0.24–1.8 van der Waals, H-bond, charge transfer
[55] [58]
Mxenes
– – 10− 6-2500 [10] – charger transfer, coordination, H-bond
[63]
2D MOFs
inexpensive and effective method, which can be used for the mass
Table 2
preparation of GO method. The surface of RGO retains some of its
Comparison of the advantages and disadvantages of the four preparation
functional groups and has semiconductor properties, therefore it is
methods for graphene.
suitable for using as gas sensitive material. However, the dispersion in
Methods Advantages Disadvantages
aqueous solution is poor and easy to agglomerate, which affects the
ME [9,48] Low cost, simple process The prepared film is not conductivity and film-forming characteristics.
uniform, which is not easy to
produce in macro scale
2.1.2. Research status of graphene gas sensors
CVD [48–50] Large area growth, high High cost, complex process
quality, controllable layers
and adjustable band gap (1) Pristine graphene-based gas sensors
Epitaxial growth Large area and high-quality High cost, it is difficult to
[51] monolayer graphene was control the surface
Graphene has been widely used in the field of gas sensing. Gas sensor
obtained morphology and the
preparation temperature is promotes wide application of graphene materials, which provides new
high ideas for the theoretical and experimental study of graphene devices. In
Chemical Low cost, high output, simple In the process of oxidation and 2007, the team of Novoselov first reported on graphene materials
oxidation operation and it is easy to intercalation, the formation of applicating in gas sensor [21]. Graphene single crystals with the size of
exfoliation modify the functional groups defects and functional groups
about 10 μm were prepared by M-ME on the surface of oxidized sillicon
[52] such as hydroxyl group and affects the conductivity of
carboxyl group on go surface graphene substrate, and then graphene-based sensor was fabricated via depositing
the graphene crystals on Au/Ti electrode by electron beam lithography.
The graphene-based sensor can detect 1 ppm several gases (NO2, NH3,
The graphite powder is first oxidized to GO by CVD, and then the GO CO and H2O), as shown in Fig. 2a. It is found that when the target gas are
layer is oxidized by ultrasonic treatment. The OCFGs are finally removed adsorbed on graphene surface, the carrier concentration of graphene
by thermal reduction, chemical reagent reduction and photoreduction to will change, resulting in a change of resistance. The resistivity of the
obtain RGO [53]. instrument changes with different adsorbed gases. This study proposes a
Graphene prepared by different methods has different properties new idea for further development of graphene gas sensors. In addition,
[54], as shown in Table 2. Although the process of preparing graphene Leenaerts et al. [55] researched the physical adsorption behavior of
by ME is simple and cost-effective, the graphene prepared by this NH3, NO2 and CO on surface of graphene nanosheets (NSs). The calcu
method is not uniform in thickness and is not easy to be produced in lation results of DFT show that gas adsorbed on the pristine graphene
large scale. Although excellent graphene is prepared by CVD and surface act as dopants, resulting in the obvious change in the local
epitaxial growth method, the process of preparing graphene by CVD carrier concentration.
method is complex and cost-effective. The conditions of preparing gra However, the pristine graphene has almost no dangling bonds on its
phene by epitaxial growth method are severe and require high tem surface, which makes it difficult for the target gas to be chemisorbed. As
perature, so it is more difficult to control the number and thickness of a result, pristine graphene gas sensor reacts very slowly and cannot
graphene layer. Chemical oxidation exfoliation method is an completely return to the initial state after adsorption of gas. The long
4
Fig. 2. (a) Changes in resistivity, ρ, at zero B caused by graphene’s exposure to various gases with 1 ppm [20]. Reproduced with permission from ref. 20. Copyright
2007, Nature Publishing Group.; (b) Photographs of a fabricated all-graphene gas sensor on PI substrate (left); Response and recovery curves of the unpatterned
graphene sensor to 5 ppm NO2 at different temperatures (top right) and comparison of the response curve at 180 ◦ C with that of the patterned graphene sensor at 60 V
(bottom right) [57]. Reproduced with permission from ref. 57. Copyright 2015, American Chemical Society.; (c) Responses of Ar-irradiated graphene gas sensor for
CO, NH3 and NO2 gas flow with different irradiation energy [58]. (d) Schematic draw of the fabrication process for the ozone-treated graphene gas sensor, (e) The
resistance changes of the OTG (red) and pristine graphene (black) sensors (NO2 concentration in the range from 200 ppm to 200 ppb). The inset shows the correlation
between percentage response and concentrations, which is in agreement with the Langmuir adsorption model [59]. Reproduced with permission from ref. 58.
Copyright 2019, Elsevier.; ref. 59. Copyright 2012, Elsevier. (For interpretation of the references to colour in this figure legend, the reader is referred to the Web
version of this article.)
response and recovery time of gas sensor based on pristine graphene can NO2 and CO gases have been greatly improved in Fig. 2c [59].
be attributed to the slow adsorption process of the pristine graphene at In order to enhance performance of pristine graphene-based sensors,
RT [56,57]. Under the circumstances, some researchers suggest that a promising solution is to functionalize the pristine graphene consists of
response of pristine graphene gas sensor is improved by external exci introducing defects and functional groups. In 2012, Chung et al. pro
tation (heating and ion beam irradiation). Kim et al. proposed flexible posed to improve sensing performance of graphene NO2 sensor by
self-active NO2 sensor based on graphene [58], the response and re adding plenty of OCFGs into graphene by ozone treatment [60]. The
covery characteristics of which were increased by increasing the bias fabrication process of ozone treated graphene (OTG) NO2 sensor is
voltage and heating temperature of the sensor (Fig. 2b). Yeo et al. pro shown in Fig. 2d. The experimental results show that the response value
posed to irradiate graphene with ion beam [59], and compared with the and response time of OTG sensor are significantly improved. The
pristine graphene, the responses of Ar-ion irradiation graphene to NH3, response of the OTG sensor is twice as high as that of the pristine
5
graphene sensor to 200 ppm NO2 at RT (Fig. 2e). The contact between number of OCFGs can be changed by chemical reduction of GO and its
graphene, B-or N-doped graphene, defective graphene and CO, NO, NO2, conductivity can be increased. Thus, RGO is a typical material that
NH3 were studied by Zhang and his group [61]. This work establishes conducts electricity well. Gas is adsorbed on RGO and then electrons
that the response of gas sensors is largely improved by adding dopant or transfer between gas and RGO, resulting in the change of carrier con
defect. In addition, Bo et al. reported the adsorption behaviors of NO2 centration in RGO body. According to this principle, many researchers
and H2S on Ni, Pd and Pt decorated graphene [62]. The results of DFT have carried out the research work of RGO based RT gas sensors. As
calculation show that the metal decorated graphene has strong chemi early as 2009, the research team led by Professor Chen suspended GO on
sorption on gas molecules, in particular, Ni decorated graphene has Au electrode to form GO film, after heat treatment at 100–300 ◦ C in
highly sensitivity to NO2 (Fig. 3a). Its adsorbing energy and charge argon, GO was partially reduced to RGO, which was made to realize
transfer are 7–10 times and 3–10 times higher than those of the pristine detection of NO2 (Fig. 3b–d) [68]. Subsequently, the team prepared RGO
graphene, singly. by reducing GO by hydrazine. Then, RGO was used as the gas sensitive
layer and the conductive channel of the source and drain, and silicon
(2) RGO-based gas sensors sheet was used as the gate to construct a field effect transistor (FET)
sensor (Fig. 3e and f). Compared with the previous thermal RGO based
The chemical inertness and zero band gap of pristine graphene limit sensor, the response of RGO treated by hydrazine sensor toward 100
its application in electronic component. To this end, GO was synthesized ppm NO2 is remarkably improved by 360% [69]. Nonetheless, the
by Hummers’ method, which was applied to fabricate gas sensors [63]. pristine RGO gas sensor has disadvantages, including low response, long
Comparison of pristine graphene and GO suggests that GO is strongly response time and incomplete recovery behavior (Fig. 3c and g).
oxygenated with sufficient OCFGs on its defect region [64,65], which act Numerous experiments have established that surface functionalization,
as reactive sites for gas adsorbing [66]. Nonetheless, GO has poor con heteroatom dopant, metal and metal oxide modification, conductive
ductivity with respect to conjugated electronic structure disturbed by polymer composite, laser irradiation and other factors have significant
OCFGs, impeding its application in electronic component [67]. The influence on gas sensing performance of RGO, which can solve the above
Fig. 3. (a) Optimized structure, electron density map and DOS of graphene decorated with Ni atom (left); Dashed line and solid line present the DOS of pristine
graphene and metal decorated graphene, respectively. Electron density and isosurface map of difference electron density of NO2 adsorption on the Ni/graphene
surface (middle); DOS of Ni/graphene with NO2 adsorption (labeled by (Ni/graphene)after-ads) and without NO2 adsorption (labeled by (Ni/graphene)before-ads), PDOS
of NO2 molecule and Ni atom after gas adsorption (right) [61]. Reproduced with permission from ref. 61. Copyright 2019, Elsevier.; (b) RGO based sensor, (c)
Response and recovery curves of GO after annealing in Ar at 200 ◦ C to 100, 50, and 25 ppm NO2. (d) GO after annealing in Ar at 200 ◦ C and 300 ◦ C to 100 ppm NO2
[67]. Reproduced with permission from ref. 67. Copyright 2009, American Institute of Physics.; (e) Schematic of the RGO device with an FET platform, (f) SEM image
of a sensing device composed of RGO platelets that bridge neighboring Au fingers, (g) Dynamic response curve of RGO sensor to 100 ppm NO2 [68]. Reproduced with
permission from ref. 68. Copyright 2011, American Chemical Society.
6
problems of pristine RGO based gas sensor. surface of materials with respect to larger specific surface area and the
pore structure. The team of Huang in Northwestern University etched
(3) Functionalized RGO based gas sensors GO NSs with 200 ◦ C steam in a sealed container to obtain PRGO with
defective structures (Fig. 4c). In contrast to the untreated RGO, the
In 2014, Kim et al. from Hanyang University prepared RGO gas sensitivity of PRGO to 100 ppm and 250 ppm NO2 was increased by two
sensor by reducing it with hydrazine at 150 ◦ C (Fig. 4a) and found that orders of magnitude (Fig. 4d) [71]. Yuan et al. used the solution etching
the number of OCFGs in RGO increased under electron beam irradiation. method to mix a certain amount of GO solution with H2O2 solution
The OCFGs could be used as active centers for adsorption of NO2. As (30%) to obtain GO with porous structure (PGO), and then reduced PGO
shown in Fig. 4b, the RGO films irradiated by 100 and 500 kGy electron with hydrazine to obtain PRGO. It can be seen from Fig. 4e that the pore
beams have a higher response value than that of those without irradi volume of PGO is significantly larger than that of GO, and the specific
ation [70]. Although the method of electron beam irradiation does surface area of PRGO is nearly three times that of RGO. Obviously,
address the problem of low sensitivity of pristine RGO based gas sensor compared to RGO, PRGO has better gas sensitivity to NO2 (Fig. 4f) [72].
to a certain extent, the treatment of irradiation process is complicated, 3D structure can increase the contact area between the sensitive mate
which is not conducive to the development of sensor portability. rial and gas, and active sites of sensing material, thereby improving the
The sensitive material is the major part of the sensor. The method of gas sensing characteristics. Fig. 4g summarized Lee et al. from Sung
improving the response and recovery properties of RGO sensor are kyunkwan University spin coated SU-8 2050 PR onto SiO2/Si substrate
attracting widespread interest. Firstly, some researchers propose to and heat-treated to prepare 3D SU-8 microcolumn. Then GO solution
prepare RGO with porous structure (PRGO) by chemical method. The was adsorbed on the microcolumn, and finally reduced by hydrazine
gas molecules can accelerate the diffusion and desorption rate on the vapor to obtain 3D RGO. In contrast to 2D RGO, RGO with 3D structure
Fig. 4. (a) A schematic of sensor fabricated with RGO films, (b) The response and recovery curves of unirradiated, 100 kGy-irradiated and 500 kGy-irradiated sensors
to 10 ppm NO2 [69]. Reproduced with permission from ref. 69. Copyright 2014, Elsevier.; (c) TEM images of suspended GO sheets before and after being steamed, (d)
Responses of thermally RGO and the steamed GO sheets upon exposure to NO2 [70]. Reproduced with permission from ref. 70. Copyright 2011, American Chemical
Society.; (e) BJH pore size distribution of freeze-dried GO and PGO, (f) Comparison between the normalized conductance change of PRGO and RGO-based sensors
upon 500 ppb NO2 [71]. Reproduced with permission from ref. 71. Copyright 2018, Elsevier.; (g) Schematic structure of both 2D and 3D devices and cross-section of
3D device, (h) Response and recovery of RGO sensors towards 5 ppm NO2 and sensing response of RGO sensors towards 40 ppm NH3 [72]. Reproduced with
permission from ref. 72. Copyright 2015, WILEY-VCH.; (i) SEM image showing the interior 3D porous nanostructures of RGOH, (j) Comparison between the response
of 3D RGOH and that of 2D RGO NSs to NO2 with different concentrations [73]. (k) High-magnification SEM images of the lyophilized 3D crumpled NA-RGO
nanosheets, (l) Response comparison of 3D-CNN, NA-RGO, and RGO sensors toward 10 ppm of NO2 [74]. Reproduced with permission from ref. 73. Copyright
2015, American Chemical Society.; ref. 74. Copyright 2017, American Chemical Society.
7
has higher response to NH3 and NO2 (Fig. 4h), and lower detection limit rich OCFGs exist on the surface of GO. Hence, GO has good dispersion in
of NH3 at RT [73]. In addition, Professor Norford from Nanyang Tech water and other solvents. Metal cations (such as Sn4+, Zn2+, In3+, etc.)
nological University and Professor Wang from Beijing University also interact with GO by electrostatic adsorption, and then metal oxide
prepared 3D RGO by hydrothermal synthesis and freeze-drying tech decorated RGO composites are synthesized by hydrothermal synthesis,
nology (Fig. 4i and k), respectively [74,75]. Comparatively, 3D RGO has solvent heat treatment and chemical deposition methods [54].
higher sensitivity to NO2 than that of RGO (Fig. 4j and l). The performances of some metal oxide decorated RGO gas sensors
are seen in Table 4. SnO2 is a kind of n-type oxide extensively used.
(4) Gas sensors based on RGO based composites When SnO2 nanocrystals are decorated on the surface of RGO, on the one
hand, the surface area and the number of active sites of composite in
The combination of RGO with metal, metal oxide and polymer has crease, which could improve the adsorbing capacity of gas on material.
been proved to be a straightforward and effective strategy to realize On the other hand, the heterostructure is formed between RGO and
high-performance gas detection and further improve the sensing per SnO2, which promotes the electron conduction between them, changes
formance of RGO sensors. These RGO based hybrid nanostructures the Fermi level position of RGO, and further improves the conductivity
possess exciting properties due to the different functions and synergistic of SnO2-RGO [54]. Zhang et al. successfully prepared SnO2 NPs and RGO
effects between the contained components, which greatly changes the (SnO2-RGO) composites by hydrothermal treatment of GO dispersion,
electronic properties of RGO [76]. which were used to detect NO2 at 50 ◦ C. The results illustrate that the
It is generally accepted that noble metal modified RGO complexes response of SnO2-RGO to 5 ppm NO2 is approximately 3.31, which is
have superior gas sensing performance, mainly because of the syner much higher than that of RGO (1.13) [82]. In 2019, Kooti et al. also
gistic effect of catalytic activity of noble metal and conductivity of RGO synthesized SnO2 nanorods and RGO (SnO2 NRs-RGO), and then were
at RT. The adsorbed target gas is catalyzed on the surface of noble metal, print screened on Al2O3 substrates for methane sensors. At 150 ◦ C,
and electrons captured from the catalytic reaction are transmitted to response value of SnO2 NRs-RGO to 1000 ppm CH4 is 24.9%, which is
electrode through RGO, so that the sensor has striking changes in elec 600% higher than that of pristine SnO2 NRs [83]. Chu et al. fabricated
trical signals [25]. The performances of several noble metal decorated SnO2-RGO sensor, which was used to detect the decomposition com
RGO based gas sensors are compared in Table 3. Among them, Hirsch ponents of sulfur hexafluoride (SF6) such as H2S and SOF2. The results
et al. used PdCl2 and K2PtCl4 as metal precursors to load Pd and Pt illustrate that SnO2-RGO sensor has better response to 100 ppm H2S and
nanoparticles (NPs) on RGO NSs by wet chemical method. The response 10 ppm SOF2 at 125 ◦ C than that of pristine RGO sensor, with the
values of Pd-RGO and Pt-RGO to 25 ppm NO2 were about 1.65 and 1.15 response values of 33.02% and − 3.24% (the response values of the
at 85 ◦ C [77]. Johnson and his colleagues synthesized a hybrid of pristine RGO sensor are 5.97% and 1.45%) [84]. In addition, Li et al.
multilayer graphene nanobelts (NBs) and NPs on a micromachined prepared SnO2-RGO with 3D structure as by hydrothermal and lyophi
porous substrate to detect H2, and the response value of Pd-RGO is lization strategy, and its response to 100 ppm NO2 is about 1.05 [85].
~55% for 40 ppm H2 [78]. Li et al. deposited RGO with physically Liu et al. subjected a solvothermal treatment of GO with Sn4+, and then
absorbing Pd NPs on its surface on CVD graphene-coated Ni electrodes freeze drying. A 3D RGO aerogel-supported SnO2 NPs was prepared for
to detect NO. Compared with RGO, Pd-RGO has higher sensitivity and detection of NO2. The response of this aerogel to 10 ppm NO2 is about
the minimum detectable level (2 ppb NO) [79]. Luan et al. impregnated 1.14 [86].
the commercial polyurethane (PU) sponge block in the mixed solution of In the same way, other metal oxides and RGO composites can also
Ag nanowires (NWs) and RGO, and then dried them to obtain flexible Ag detect target gases at RT [87]. For instance, Zhang and Liu et al. con
NWs-RGO. The response of Ag NWs-RGO to 50 ppm NO2 was about 1.18 structed a NO2 gas sensor using ZnO-RGO as sensing materials. The
at RT under 60% tensile strain [80]. In addition, Chen et al. used su response value of ZnO-RGO to 5 ppm NO2 is about 1.26 [88]. Galstyan
pramolecular self-assembly method to obtain naphthalene sodium sul et al. prepared a nanostructured ZnO-RGO sensor for the detection of
fonate modified RGO (NA-RGO), and then loaded Ag NPs on NA-RGO to VOCs (C2H5OH and CH3COCH3). The experimental results show that the
obtain Ag–Na-RGO [81]. The ability of sulfophenyl to attract electrons response of ZnO-RGO sensor to 100 ppm ethanol and acetone (120% and
and the catalysis of Ag make Ag–Na-RGO based sensor have good RT 140%) is apparently higher than that of ZnO sensor (55% and 35%)
sensitive properties, and its response value to 10 ppm NO2 is 2.8, while [89]. In2O3-RGO were synthesized using hydrothermal method by Gu
that of RGO and NA-RGO is only 1.4 and 2.0 for the same concentration et al., which has high response (8.25) and short response time (240 s)
of NO2. and recovery time (1440 s) to 30 ppm NO2 at RT [90]. Yang et al. pre
Metal oxides (e.g., SnO2, ZnO, In2O3, Co3O4 and others) have been pared In2O3 cubes-RGO composites. The response value of In2O3
widely used in the field of gas sensor. Many researchers have tried to cubes-RGO to 5 ppm NO2 is about 1.61 [91]. In 2019, Sakthivel et al.
prepare metal oxide and RGO composites. RGO can improve electrical synthesized NH3 sensors based on CuO and RGO (CuO-RGO) by
conductivity at RT, and metal oxides with nanostructures can prevent surfactant-free hydrothermal treatment. The response value of
the agglomeration of RGO NSs to a certain extent. In addition, p-n or p-p CuO-RGO sensor to 600 ppm NH3 is 13 near RT (30 ◦ C) [92]. Yin et al.
heterostructures exists at the interface region between RGO (p-type) and prepared a sensor based on CuO-RGO to detect H2S. At 100 ◦ C, response
metal oxide (n-type or p-type), forming a space charge depletion region, of CuO-RGO to 5 ppm H2S is 28 [93]. In addition, Liu et al. prepared a
which can provide an effective way for charge transfer and increase the H2S sensor prepared by Co3O4-RGO, of which response value to 50 ppm
activity of gas adsorption. Therefore, metal oxide decorated RGO shows H2S at 50 ◦ C is 30.6, and H2S gas concentration is as low as 0.1 ppm [94].
excellent gas sensing properties. Generally, the negative charges and Su et al. fabricated a WO3-RGO sensor for detecting NO2 by one-pot
Table 3
Comparison of the sensing performance of noble metal decorated RGO based gas sensors.
Materials Target gases Concentration (ppm) Response value Response and recovery time (s/s) Limit of detection (ppm) Ref.
Pd-RGO NO2 25 ~1.65 − /− 25 [76]

Pt-RGO NO2 25 ~1.15 − /− 25 [76]
Pd-RGO H2 40 ~55% − /− 40 [77]
Pd-RGO NO 0.002 ~4% 240/1000 0.002 [78]
Ag NWs-RGO NO2 50 1.18 − /− 5 [79]
Ag–Na-RGO NO2 5 1.74 600/2400 5 [80]
8
Table 4
Comparison of the sensing performance of metal oxide decorated RGO based gas sensors.
SnO2-RGO NO2 5 ~3.31 − /− 1 [81]

SnO2-RGO CH4 1000 24.9% 369/519.8 1000 [82]
SnO2-RGO H2S 100 33.02% 209/900 3 [83]
SnO2-RGO SOF2 10 − 3.24% 255/330 1 [83]
(3D) SnO2-RGO NO2 100 1.05 300/- 14 [84]
(3D) SnO2-RGO aerogel NO2 10 1.14 − /− 10 [85]
ZnO-RGO NO2 5 1.26 165/499 1 [86]
ZnO-RGO ethanol 100 120% − /− 100 [87]
ZnO-RGO acetone 100 140% − /− 50 [87]
In2O3-RGO NO2 30 8.25 240/1440 5 [88]
In2O3 cubes-RGO NO2 5 1.61 ~180/- 1 [89]
CuO-RGO NH3 600 13 16/80 6.5 [90]
CuO-RGO H2S 5 28 20/920 1 [91]
Co3O4-RGO H2S 50 30.6 − /− 0.1 [92]
WO3-RGO NO2 5 8.69 540/1080 1 [93]
ZnO nanorods-RGO NO2 1 2.19 75/132 0.05 [94]
Co3O4-RGO NO2 60 5 − /− 60 [95]
Pt–SnO2-RGO methanol 40 60.1 6/21 10 [96]
Pd–MnO2-RGO methanol 100 ~92.52% 11/16 5 [97]
In–SnO2-RGO NO2 100 11 400/- 1 [98]
NiO–SnO2-RGO NO2 60 62.27 ~220/~835 5 [99]
RGO-CNTs-SnO2 NO2 5 2.53 8/77 1 [100]
AgNPs/SnO2/RGO NO2 5 2.17 49/339 1 [101]
polyol process. The response value of this WO3-RGO sensor to 5 ppm gas sensing characteristics [96]. Professor Li from Dalian University of
NO2 is 8.69 at RT [95]. To obtain outstanding RT gas sensing properties, Technology fabricated a Co3O4-RGO based sensor, which has good
a lot of researchers have focused on controlling the grain size and sur sensitivity to NO2 for two reasons. On the one hand, the intercalation
face morphology of sensing materials. For example, Xia et al. have effect of Co3O4 NPs between RGO layers increases the surface area of the
grown ZnO NRs in situ on RGO, compared with monomer (ZnO NRs or composite; on the other hand, the strong coupling between cobalt and
RGO), ZnO-RGO has a higher response to NO2 at RT. Under the com oxygen in graphene makes it easier for cobalt and oxygen to bond
bined action of good charge transfer capacity of RGO and super (Co–O). Co3+ can be used as an additional adsorption center for NO2,
adsorption capacity of ZnO NRs for NO2, the composite shows excellent and electrons can be indirectly extracted from graphene and transferred
Fig. 5. (a) Schematic illustration of preparing RGO/porous PEDOT nanocomposite, (b) Gas sensitivity of different devices with RGO, RGO/PEDOT and RGO/porous
PEDOT layer as sensing layers to 20 ppm of NO2, the inset picture is the RGO/porous PEDOT covered interdigitated electrode [102]. Reproduced with permission
from ref. 102. Copyright 2014, American Chemical Society.; (c) Responses of 3D RGO and 3D RGO/PANI based sensors to NH3 at different concentrations from 100 to
600 ppm [103]. Reproduced with permission from ref. 103. Copyright 2020, IOP Publishing Ltd.; (d) Responsivity as a function of weight ratio of PANI/rGO in
PANI-rGO NH3 gas sensors operated at room temperature under 15 ppm NH3 environment and about 0% relative humidity. Inset listed responsivity recovery time of
PANI-rGO NH3 gas sensors with various weight ratios of PANI/rGO [104]. Reproduced with permission from ref. 104. Copyright 2019, Elsevier.; (e) The response and
recovery curves of the sample at different laser power of 0, 10, 40, 70 and 100 mW [108]. Reproduced with permission from ref. 108. Copyright 2016, Royal Society
of Chemistry.; (f) Gas sensing property of rGO/SnO2 sensor to 3 ppm NO2 from dark to UV light irradiation with different intensities, (g) Gas sensing property of
rGO/SnO2 sensor to 30 ppm SO2 from dark to UV light irradiation with different intensities [109]. Reproduced with permission from ref. 109. Copyright
2019, Elsevier.
9
to NO2 through bonded oxygen atoms, thus resulting in more reduction These TMDs sensors are applied onto national defense, security and
of device resistance [97]. For the sake of improving the sensitivity of Internet of Things applications [114]. The synthetic route of TMDs is the
metal oxide decorated RGO to detect target gases at RT, some re primary factor to determine the final chemical, structural and
searchers prepared ternary RGO composite nanomaterials, such as morphological properties of the active materials [26], such as CVD
Pt–SnO2-RGO [98], Pd–MnO2-RGO [99], In–SnO2-RGO [100], NiO–S process [115], liquid-phase exfoliation (LPE) [116], M-ME [117], wet
nO2-RGO [101], RGO-CNTs-SnO2 [102] and AgNPs/SnO2/RGO [103]. chemical synthesis [118], mechanical cleavage method [119], electro
Compared with binary RGO composite nanomaterials, the sensitivity of chemical exfoliation using Li-intercalation and pulse laser deposition
gas sensors is further improved by using the synergy of the three. [120]. Among all these preparation methods, CVD is the most common
The decoration of RGO with polymers has also been proved to be a method to synthesize pure, single layer and high crystal TMDs [121].
resultful strategy to improve sensing performance of graphene gas sen The process of CVD is the co-evaporation of metal oxides and sulfur
sors, e.g., Yang et al. synthesized porous poly (3, 4-ethylenedioxythio element to grow 2D TMDs, which leads to gaseous reactions and then the
phene) (PEDOT) on RGO film to detect NO2 (Fig. 5a). The response preparation of 2D TMDs on an appropriate substrate [28]. Numerous
value of PEDOT/RGO to 20 ppm NO2 is 41.7%, and response/recovery TMDs sensors fabricated by various preparation methods have reported
time is about 175 s and 70 s, as demonstrated in Fig. 5b [104]. Tohidi (Table 5). For example, Zhao et al. prepared the MoS2 on flexible PI films
et al. prepared 3D RGO/polyaniline (PANI) hybrid by hydrothermal by CVD method at 200 ◦ C (Fig. 6a). The flexible sensor showed a higher
method to detect NH3 at RT, which has a significant effect on improving response to 25–500 ppm NO2 than that of NH3 in the same concentration
sensitivity and selectivity. As shown in Fig. 5c, in contrast to pure 3D range (Fig. 6b and c) [122]. Kim et al. synthesis of 2D NbS2 NSs by CVD,
RGO, the response of 3D RGO/PANI (1:1) to 100 ppm NH3 was enhanced and DFT calculations revealed that NO2 sensing properties of NbS2 can
by 44.7 times [105]. Moreover, Lee et al. prepared a PANI-RGO sensor be modified by different edge configurations depending on synthetic
by distributing PANI on surfaces of RGO NSs to detect NH3. The response conditions [123]. Besides, LPE is considered as an emerging and excel
value and recovery time of PANI-RGO to 15 ppm NH3 at RT are 13.0% lent method, which allows the production of a large number of exfoli
and 1326 s, respectively (Fig. 5d). The lowest NH3 concentration of ated NSs (with good control over the size of the sheets), making it easy to
PANI-RGO sensor (0.3 ppm) could be detected [106]. Conjugated PANI make composite materials and mixed films [124]. As shown in Fig. 6d,
manifests high gas response because of the mutual chemical trans Chen et al. prepared MoS2 nanoflakes (NFs) by LPE [125]. The Au NPs
formation of the different types of PANI. Unfortunately, it has limited functionalized MoS2 were fabricated through a facile solution mixing
chemical stability [107]. The π-π bonds bind PANI and RGO, resulting in method. Besides, wet chemical method is also used to obtaine surface
the stability of the PANI is improved [108]. Apart from this, electron modification of 2D TMDs. For example, Han et al. designed a MoS2/ZnO
transfer exists between PANI and RGO, and also improve sensitivity and hetero-nanostructure (Fig. 6e) [126]. As shown in Fig. 6f, after surface
reversibility [109]. modification by ZnO NPs, the response of MoS2/ZnO heterogeneous
nanostructures to 5 ppm NO2 is 11 times greater than that of pure MoS2
(5) RGO based gas sensors with irradiation NSs. Wet chemical synthesis includes many methods, such as hydro
thermal method, solvent evaporation method, template-assisted syn
The above methods mainly solve the problem of low sensitivity of thesis method, self-assembly method. Among them, hydrothermal
pristine RGO based gas sensors, including surface functionalization, method and solvent thermal method are the two most commonly used
heteroatom doping, the modification of metal, metal oxide, conductive methods [127,128]. In addition to the above methods, there are also
polymer and so on. Furthermore, the desire to address the problems that atomic layer deposition (ALD) technology for the production of sensing
long response time and incomplete recovery behavior of pristine RGO layer thin films and 2D nanostructures [129,130], and e-beam evapo
gas sensor should be improved. Karimzadeh et al. studied the effect of ration technology that is used to prepare metal oxide and other 2D
continuous laser beam irradiation on the sensing response of CO gas nanomembranes [131,132].
sensor, and compared the conductance of RGO based gas sensors before
and after irradiation [110]. The experimental results reveal that RGO 2.2.2. Research status of TMDs gas sensor
based gas sensor with laser irradiation has a faster response to CO gas
than that of RGO sensor without irradiation, and the sensitivity increases (1) MoS2-based gas sensors
with the increase of laser power (Fig. 5e). Such excellent sensing prop
erties are related to the removal of OCFGs during laser irradiation. The MoS2 is one of typical representatives of chemical sensing TMDs
method of laser irradiation does improve the problem of long response owing to its unique physical and chemical features, including the
time of pristine RGO based gas sensor, but the recovery time of the layered band gap, high surface volume ratio and high adsorption
sensor becomes slower after laser irradiation. Subsequently, Li et al. properties. MoS2 has 2D structure similar to graphene, with the layers
reported the gas-sensitive properties of RGO/SnO2 sensors under stacked on top of each other to form a block (Fig. 6g) [133]. These layers
different UV irradiation intensities [111]. As shown in Fig. 5f and g, the are held together by VDWFs [134]. Each 2D crystal layer of MoS2 has a
RGO/SnO2 sensors exposed to UV light has a more complete response hexagonal arranged molybdenum atomic plane sandwiched between
and recovery behavior to NO2 and SO2. The sensitivity also increases two hexagonal arranged sulfur atomic planes, and the covalently bonded
with the increase of UV intensity. Drmosh et al. proposed that the S–Mo–S atoms are arranged in a triangular prism to form a hexagonal
Au/RGO/ZnO sensor has better selectivity and sensitivity for H2 detec crystal structure [134]. It has been reported in the literature that the
tion at RT with UV irradiation, which is due to the electron-hole pairs surface structure of MoS2 is different from that of metal oxides and the
excited by UV irradiation [112]. In addition, Hassinen et al. prepared a mechanism of gas sensitivity is also different. There is charge transfer
paper-based RGO sensor. With the help of UV irradiation, RGO sensor between MoS2 and NO2, which is conducive to the detection of NO2 [67,
can recover completely after responding to NO2 [113]. 135]. Cho et al. prepared layered MoS2 with atomic layer thickness by
CVD method, and explained charge transfer mechanism between MoS2
2.2. Gas sensors based on TMDs and NO2 by in-situ fluorescence spectroscopy characterization [32].
Donarelli et al. obtained MoS2 NSs by LPE and realized NO2 detection at
2.2.1. Synthesis of TMDs 150–250 ◦ C [136]. However, the problems of low response and slow
In recent years, some 2D TMDs (MoS2, MoSe2, WS2, WSe2, etc.) have response-recovery of pure MoS2-based gas sensor need to be further
generated research interest in the application of low-power and intelli solved. By modifying or functionalizing the sensor layer with noble
gent sensing owing to inherent large specific surface area, high carrier metal NPs and semiconductor materials, the sensitivity of the sensor can
mobility and its special band gap tunable semiconductor properties, be improved [137,138]. Zhang et al. demonstrated the effect of noble
10
Table 5
Comparison of the sensing performance of TMDs based gas sensors.
MoS2 NO2 500 ~300% 180/480 25 [120]

MoS2–Au acetone 120 31.6% 102/386 10 [122]
MoS2/ZnO NO2 5 30.5 40/- 0.05 [123]
Pd–MoS2 NO 2 700% − /− 0.1 [138]
Ni–MoS2 H2S 2 80% − /− 0.3 [138]
MoS2/GO triethylamine 10 9.3 18/17 1 [139]
Ag/Fe2O3@MoS2 NO2 5 202.2% 81/355 1 [140]
MoS2/SnO2 NO2 5 18.7 74/- 0.25 [141]
MoS2@In2O3 NOx 100 10.13 1/47 0.1 [144]
MoS2–Au NO2 2.5 30% 240/840 2.5 [146]
SnS2 NO2 0.5 25.4 ~840/~1050 0.1 [149]
SnS2 NH3 500 4.2 16/450 20 [150]
WS2 NO2 0.8 55.9% − /− 0.005 [158]
Au-WS2 CO 50 1.477 174/30 1 [160]
MoS2@WS2 NO2 50 26.12 1.6/27.7 0.01 [162]
WS2–ZnS NO2 5 32.5 4/- 0.01 [163]
Ni–In2O3/WS2 formaldehyde 5 ~23.5 76/123 0.015 [164]
Pt-WS2 NH3 250 ~9.5% − /− 0.05 [165]
WS2–TiO2 NH3 250 43.72% -/174.43 20 [166]
MoSe2 NH3 1 5.5% 15/135 1 [169]
Pd–MoSe2 NH3 50 7.58 130/80 5 [170]
Nb–MoSe2 NO2 3 8.03 − /− 3 [173]
Fig. 6. (a) Schematic image of the flexible gas-sensing device consisting of CVD MoS2 channels and Au/Ti electrodes. (b) Gas-sensing results for the 2D MoS2-based
flexible gas sensors consisting of MoS2 with bending upon NO2 exposure (25, 50, 100, 200, 500 ppm) and (c) NH3 exposure (25, 50, 100, 200, 500 ppm) [120].
Reproduced with permission from ref. 120. Copyright 2018, Royal Society of Chemistry.; (d) Schematic process flows for the fabrication of MoS2-based nanoflakes
and gas sensors [122]. (e) Schematic of sensing mechanisms of MoS2/ZnO to NO2 molecules, (f) Sensing response of MoS2/ZnO with different amounts of ZnO NPs at
5 ppm NO2 [123]. Reproduced with permission from ref. 122. Copyright 2019, American Chemical Society.; ref. 123. Copyright 2018, American Chemical Society.;
(g) Crystal structure of MoS2. Top view and side view of monolayer hexagonal crystal structure of MoS2 (left), Trigonal prismatic (2H) and octahedral (1T) unit cell
structures (right) [130]. Reproduced with permission from ref. 130. Copyright 2020, Elsevier.
metal doping on H2 sensing performance of MoS2 in a single molecular between H2 molecules and MoS2. Then, the band gap of Cu, Pd and Pt
layer by the first principle [139]. Doping Cu, Pd and Pt significantly doped MoS2 is increased due to H2 adsorption, resulting in the
reduced adsorption energy of gas on MoS2 and enhanced the interaction increasing of charge transfer between H2 molecule and MoS2. Xu et al.
11
explored that both Au and Pt adsorption MoS2 monomolecular mem triethylamine at 260 ◦ C. Yin et al. synthesized Ag NPs-Fe2O3@MoS2
branes have high adsorption energy by using DFT calculations [140]. In hybrids by solvothermal method [144]. The response of
addition, Xiao et al. used metal X (Fe, Co, Ni and Cu) atoms to replace S Ag–Fe2O3@MoS2 sensor to 5 ppm NO2 is ~11.8 times (17.1%) than that
atoms on MoS2 monolayer surface respectively and explored the of MoS2 (Fig. 7b). Han et al. prepared MoS2/SnO2 heterostructures to
adsorption of gas molecules based on the DFT theory [141]. For Fe, Co, solve the problem of inadequate sensitivity and poor recoverability of
Ni, Cu doped monomolecular layer MoS2 has a great adsorption effect on MOS2 gas sensor [145]. According to Fig. 7c, MoS2/SnO2 gas sensor
NO2 molecules, especially Fe doped MoS2 has a stronger adsorption presented an 18.7 response to 5 ppm NO2. Besides, the alignment di
effect on NO2. The reason that Fe doped MoS2 can effectively activate rections of MoS2 crystals can also affect gas sensing properties. Cho et al.
the adsorbed NO2 molecule. Aneesh et al. prepared Ni and Pd func studieded three MoS2 films with different alignment directions
tionalized MoS2 by hydrothermal process [142] and proved that (HA-MoS2, MHVA-MoS2, VA-MoS2) by using rapid sulfurization method
Pd–MoS2 layer showed high sensitivity to 2 ppm NO (700%) with the of CVD process [146]. Among them, the response value of VA-MoS2 NO2
minimum detection limit of 0.1 ppm, while Ni–MoS2 shows 80% sensor was five times higher than that of the other two. Jung et al. also
sensitivity to 2 ppm H2S gas. Besides, the development of hybrid synthetized VA-MoS2 layers by CVD method [147]. It is demonstrated
structures is another effective strategy for increasing large surface areas that VA-MoS2 was remarkably rich in surface exposed edge sites and
and modulating intrinsic electronic properties to improve sensitivity. abundant in dangling bonds due to its anisotropy of crystals by using
Zhang et al. prepared MoS2/GO with different mass ratios of GO to MoS2 DFT and finite element method (FEM) analysis.
by hydrothermal method [143]. As shown in Fig. 7a, the MoS2/GO-3% In addition to above methods, other methods are also studied to
sensor exhibited a response value greater than 75 towards 50 ppm improve the gas sensitive properties. 3D MoS2 NSs grew on mesoporous
Fig. 7. (a) Response stability of MoS2/GO sensors upon exposure to 50 ppm TEA operating at 260 ◦ C [139]. (b) Plots of response of the sensors to different con
centrations of NO2 ranging from 1 to 35 ppm. (MoS2 at 180 ◦ C with UV irradiation, Fe2O3@MoS2 at 150 ◦ C with UV irradiation, Ag–Fe2O3@MoS2 at 120 ◦ C without
irradiation) [140]. (c) Selectivity of MS-1.25 to 5 ppm NO2, 50 ppm NH3, and other analytes with 1% of saturated vapor concentrations, and the concentrations of 1%
saturated CH3OH, C6H5CH3, HCHO vapors equal to 1670, 380 and 1970 ppm, respectively. The inset picture is long-term stability of MS-1.25 to 5 ppm NO2 for a 4
weeks’ period [141]. (d) Proposed synthesis of the MoS2@In2O3 nanocomposite [144]. (e) Schematic illustration of the forming process of the ultra-thin WS2 NSs
[159]. (f) Illustration of different distribution situations of ZnS NSs on the surface of WS2 NSs (left). Energy band structures of WS2/ZnS heterostructure in air and the
proposed sensing mechanism of WS2/ZnS heterostructure (right) [163]. Reproduced with permission from ref. 139. Copyright 2020, Elsevier.; ref. 140. Copyright
2020, Elsevier.; ref. 141. Copyright 2019, Elsevier.; ref. 144. Copyright 2019, Elsevier.; ref. 159. Copyright 2018, Elsevier.; ref. 163. Copyright 2019, Elsevier.; (g)
Response comparison for the five sensors [164]. Reproduced with permission from ref. 164. Copyright 2020, American Chemical Society.; (h) The response of gas
sensors based on 0.44 TiO2 QDs/WS2 nanohybrids, large particle TiO2/WS2 and monolayer WS2 as a function of different concentrations of ammonia gas from 20
ppm to 500 ppm [166]. Reproduced with permission from ref. 166. Copyright 2017, Elsevier.; (i) Schematic illustration of exfoliation of MoSe2 using the
probe-sonicator [169]. (j) Comparison of gas responses of the three devices as a function of the NO2 concentration. The fitted lines follow a linear relationship
between the response and concentration at 150 ◦ C [173]. Reproduced with permission from ref. 169. Copyright 2020, American Chemical Society.; ref. 173.
Copyright 2017, American Chemical Society.
12
In2O3 (MoS2@In2O3), which were successfully prepared by Shi et al. recovery was incomplete. After the functionalization of WS2, the
(Fig. 7d) [148]. The mesoporous MoS2@In2O3 manifested a response of response of MoS2@WS2-based sensor is strikingly enhanced (26.12–50
10.3–100 ppm NOx. Liu et al. solved the problem of weak response and ppm). In contrast to pure WS2, the p-n WS2–ZnS heterostructures were
incomplete recovery of the pure MoS2 sensor at RT by decorating MoS2 proposed by Yang et al. (Fig. 7f), which showed a higher response of
with PbS quantum dots (QDs) [149]. Zhou et al. studied that Au–MoS2 32.5 to 5 ppm NO2 with a shorter response time of 4 s at RT [167].
sensor had higher response for detecting NO2 under UV irradiation, Moreover, a high sensitive HCHO sensor based on Ni–In2O3/WS2 was
complete recovery properties and good repeatability than that of in the fabricated by Zhang and his colleagues [168]. Compared with the
dark case [150]. pristine WS2, the response of the Ni–In2O3/WS2-based sensor to 0.5 ppm
formaldehyde was increased by about 10 times (Fig. 7g), which can be
(2) SnS2-based gas sensors closely connected with the doping of Ni and interfacial incorporation of
heterojunction. To solve the problem where response value is difficult to
With its advantages of high electronegativity, plenty of adsorbing recover to the initial value of WS2 based NH3 sensors at RT, Zeng et al.
sites, good stability, SnS2 has shown great application potential in the decorated WS2 NSs with Pt QDs (Pt-WS2) [169]. The response of Pt-WS2
field of gas sensor [151]. Ma et al. prepared 2D SnS2 by ultrasonic to 250 ppm NH3 was 10 times than that of WS2 NSs. Soon afterwards,
exfoliation from large single crystals [152], which has a high sensitivity Qin et al. prepared WS2 NSs decorated with TiO2 QDs (WS2–TiO2) for RT
to NH3 with 5 ppm. The NO2 sensor based on assembled SnS2 NSs was NH3 sensing [170]. As shown in Fig. 7h, the response of WS2–TiO2 to
reported by Tang and his co-workers, which manifested an excellent 250 ppm NH3 is 17 times higher than that of the pristine WS2.
response of 5.7 towards 100 ppb NO2 at 120 ◦ C [153]. However, the low Furthermore, Paolucci et al. investigated the response of the WS2-mo
sensitivity limits its application in gas sensors. Zeng et al. prepared dified RGO sensor to NO2 at dry and humid air (40% RH) at 25 ◦ C and
scalable SnS2 NSs by chemical exfoliation with the response of 4.2–500 50 ◦ C under dark and Purple Blue (PB) light (λ = 430 nm) [171]. PB light
ppm NH3 [154]. They found that the high energy defect (S-vacancy) in and heating treatment (50 ◦ C) could be significantly helpful to increase
SnS2 was beneficial to increase NH3 gas adsorption. Then, adsorption recovery baseline, adsorption and desorption rates of the sensor.
behaviors of gas molecules on S-vacancy of SnS2 monomolecular layer
were studied by Zhao et al., which provide a feasible method for (4) MoSe2-based gas sensors
developing chemical gas sensors and electronic devices [155]. Hayashi
et al. made a theoretical calculation that the natural S-vacancy in n-type Atom-thin MoSe2 consists of two Se atomic layers and one Mo atomic
SnS2 plays a vital role in HCHO detection [156]. In other words, oxygen layer clamped together by covalent bonds [67]. MoSe2 NSs exhibited
atoms separated from HCHO molecules filled the vacancy, leading to the strong absorption, high surface activity and low direct bandgap, which
generation of p-type doping in SnS2, which proved the effect of S-va led to a good application in the field of gas sensor [172]. MoSe2-based
cancy on gas-sensitive performance. Qu et al. also investigated the gas sensor could detect traces of toxic gas molecules. The liquid exfoli
interaction between gas molecules and Al/Si doped SnS2 NSs with ation technique (LET) is available to prepare MoSe2 NSs for detection of
S-vacancy using DFT modeling [157]. The results showed that the NH3 [173]. The schematic illustration of exfoliating MoSe2 by
adsorption of doped SnS2 monolayer was more favorable than that of probe-sonicator was listed in Fig. 7i. A sensor was fabricated on a quartz
undoped SnS2 monolayer. On the Si doped SnS2, the adsorbed energy substrate with predeposited silver contacts to measure the gas-sensitive
was more stable than that of Al doped SnS2, which made the gas mol properties. The MoSe2-based sensor presented good response (5.5%) to
ecules have a strong adsorption capacity on Si doped SnS2. Besides, as 1 ppm NH3 with the response and recovery time of 15 s and 135 s. By
similar to MoS2, SnS2 can improve the gas-sensitive performance DFT simulation, the experimental results consistent with theoretical
through the modification of QDs and light irradiation [158,159]. results that used to study the surface charge transfer between adsorbed
ammonia and MoSe2. Zhang et al. prepared a NH3 sensor based on
(3) WS2-based gas sensors Pd–MoSe2, which was twice more responsive to 5 ppm NH3 than pure
MoSe2 [174]. Besides, NO2 induces a variety of lung and respiratory
The structure and properties of WS2 are analogous to that of MoS2 diseases, as well as acid rain formation. Thus, a lot of researches dedi
[133]. The single-layer WS2 has a hexagonal structure. Every three pairs cated to study NO2 sensors based on MoSe2. Baek et al. prepared a FET
of S are bonded to W(S–W–S), forming a certain angle in the honeycomb NO2 gas sensor based on a multilayer MoSe2 grown by CVD, which
network [160,161]. These unique physical characteristics affected the exhibited ultra-high sensitivity (1907) to 300 ppm NO2 [175]. Chen
gas sensing performance of WS2. The group of Colomer used et al. exfoliated bulk MoSe2 into NSs by LET. The response of this MoSe2
aerosol-assisted CVD (AA-CVD) method to synthesize 2D WS2 NSs for based sensor to 10 ppm NO2 (1500%) was 18 times higher than original
ultra-sensitive and unprecedented detection of 5 ppb NO2 for the first bulk MoSe2 [176]. Choi et al. added Nb atoms to 2D MoSe2 and then
time [162]. Then, ultra-thin WS2 NSs with 3D wall-like structure were synthesized MoSe2 hybrids with different Nb doping concentrations
synthesized by Xu et al. [163]. The corresponding growth mechanism [177]. As shown in Fig. 7j, the NO2 response of Nb doped MoSe2 ob
diagram of these WS2 NSs was demonstrated in Fig. 7e. The response is tained after a plasma enhanced ALD cycle was about 8 times more
9.3% for testing 100 ppb NO2 at RT. High performance WS2 based sensitive than that of pure MoSe2.
sensors were obtained by some optimization strategies, including
modifying or functionalizing the sensor layer with noble metal NPs, (5) other TMDs-based gas sensors
constructing heterogeneous junctions, doping QDs and light illumina
tion. Kim et al. prepared a flexible CO sensor based on Au-2D WS2 NFs Some other TMDs (for example VS2, MoTe2 and WSe2) have also
(Au-2D WS2) [164]. Although Au-2D WS2 sensor was bent 1000 times, been used for gas sensor (Table 6) [178]. Zhang et al. successfully
its sensing properties remained essentially the same. Apart from this, UV assembled the MoS2 NSs on the porous VS2 (P-VS2) scaffold and pre
irradiation technique was used to improve response [165]. The Au-2D pared the MoS2/VS2 heterostructure (Fig. 8a) [179]. Their gas sensitive
WS2 sensor with an irradiation time of 15 s showed the best response characteristics were dissected by using QCM technology. DFT calcula
to CO. tions and QCM experimental results showed that MoS2/VS2 based sensor
In order to solve the problem of incomplete recovery and low had an impressive affinity for NH3 and a higher adsorption capacity than
sensitivity, construction of 2D TMDs heterostructure is an effective way the original MoS2 or P-VS2 sensors. MoTe2 is a new addition to 2D TMDs.
for improving sensing performance. Shi et al. synthesized a hetero Unlike other TMDs, the band gap of MoTe2 is less than 1.0 eV [180].
junction of MoS2@WS2 by one-pot hydrothermal reaction [166]. The Feng’s group prepared MoTe2 NFs by ME and improved the sensing
response of the original MoS2 NSs to NO2 was low (2.7–50 ppm) and the performance of MoTe2 gas sensor with continuous light illumination
13
Table 6
Comparison of the sensing performance of other 2DMs based gas sensors.
BP NO2 1 ~80% ~70/- 0.1 [194]

Pt/BP H2 10 500% − /− 10 [195]
Pt/BP NOx 10 2.19 1.93/- 0.03 [196]
g-C3N4 ethanol 50 182.4 115/121 0.5 [199]
α-Fe2O3/g-C3N4 ethanol 100 7.76 7/30 50 [200]
Ni–SnO2/g-C3N4 acetone 10 142.5 49/26 0.00138 [201]
Ti3C2TX NH3 100 0.21 − /− – [203]
Ti3C2TX acetone 100 0.075 − /− 9.27 [203]
Mo2CTX MXene toluene 140 2.81 − /− 0.22 [205]
Mg-MOFs NO2 10 1.24 167/92 1 [211]
In2O3 PHRs Cl2 10 2256 38/13 0.0032 [212]
BN CH4 100 780% 10/15 – [213]
BN O2 100 150% 70/100 – [213]
Pt-BN propane 1500 – 1.35/0.6 – [214]
[180]. The research results found that the response to NH3 was appar layers of phosphorene NSs.
ently increased by more than 25 times under 254 nm UV-light. In
addition, Wu et al. also used the same method of UV-illumination to (3) Synthesis methods of g-C3N4
improve the gas sensitive performance of MoTe2 sensor (Fig. 8b) [181].
In contrast to the sensitivity of NO2 sensor under dark conditions, the Chemical-etching method is the most common method for fabri
sensitivity was significantly increased by an order of magnitude under cating g-C3N4, which is widely used in porous nanostructures. The
254 nm UV-light (Fig. 8c). Panigrahi et al. used DFT calculations to show porous ultra-thin g-C3N4 NSs by long-term thermal treatment of g-C3N4
that the substitution of Sb for Te in MoTe2 not only enhanced the binding bulk in an oxidizing atmosphere [189]. In addition, solvothermal
energy, but also caused significant changes in electronic properties and method can also be available to obtain g-C3N4 NSs. Han et al. synthe
work functions [182]. MoTe2 is indeed an ideal material for gas sensing sized g-C3N4 NSs by liquid exfoliation of g-C3N4 bulk [190]. Notewor
of NH3, NO, NO2 and other gases. thily, dicyandiamide as the precursor was calcined and thermal
polymerization occurred to form g-C3N4 bulk. g-C3N4 bulk was dispersed
2.3. Gas sensors based on other 2DMs in isopropanol mixed solvent. And, g-C3N4 NSs were obtained by sol
vothermal treatment. Some studies have proved that the longer the
2.3.1. Synthesis methods of other 2DMs for gas sensors such as BP, exfoliation time, the thinner the g-C3N4 NSs obtained.
phosphorene, g-C3N4, Mxenes, MOFs and BN
(4) Synthesis methods of MXenes
(1) Synthesis methods of BP
Selective extraction one or more elements from a material can
BP is generally synthesized by three methods: ME, LPE and CVD. At release 2D structures. Among them, selective extraction of A from MAX
first, people used scotch-tape to obtain BP NSs by ME from bulk BP phases is an effective method to synthesize 2D MXenes. The most widely
crystals. Although this method is simple, the size of obtained BP NSs is reported synthesis methods of MXenes are wet-chemical etching in HF
inhomogeneous and the production yield is extremely low [183]. In solvent. The surface functional groups (-O, –F, or –OH) are provided,
2017, Zhu and his colleagues synthesized BP NSs by ball milling BP bulk which are represented by Tx in Mn+1XnTx. There remains a need for an
using solid-state mechanochemical method [184]. Additionally, BP bulk efficient etching that can break the strong chemical bonds between A
is added to solvent, and then ultrasound-assisted stripped to obtain and M in MAX phases apart [191].
monolayer BP NSs. The yield and quality of BP NSs are bound up with
solvent [183]. The experiment demonstrated that NMP is the optimal (5) Synthesis methods of MOFs
solvent, which can provide high yield of BP dispersions [185]. The
synthesis of BP by CVD method means that the red phosphorus (RP) The different layers of 2D MOF are usually in contact by hydrogen
powder or bulk BP is heated at high temperature to grow amorphous RP bonding and VDWFs. These bonding can be broken by ultrasonic exfo
film on the silicon substrate, and then the RP thin film is transformed liation method to prepare 2D MOFs. Espallargas et al. proposed that ME
into BP NSs under high temperature and high pressure [186]. Although can be used for almost all 2DMs [192]. Langmuir-Blodgett (LB) method
large-area layered BP NSs can be obtained using the CVD method, the is a good approach to obtain large-area and thin 2DMs on liquid surface.
progress is still at an early stage, and more efforts are needed to syn 2D MOFs are prepared by dispersing the monomers of MOFs on the
thesize thinner BP NSs [183]. surface of the liquid and injecting a solution of metal ions into them
[193]. This method can be used to prepare single or multi-molecule
(2) Synthesis methods of phosphorene MOFs.
Phosphorene refers to the monolayer form of BP. It is also synthe (6) Synthesis methods of BN
sized by ME and LPE. The monolayer phosphorene NSs can be synthe
sized by a scotch tape-based ME to peel thin flakes from BP bulk and BN can be synthesized by ultrasonic exfoliation and CVD method. In
then attached them to the silicon wafer covered with thermally grown 2011, Coleman’s team dispersed BN powder in isopropanol for ultra
SiO2 layer [187]. Although ME method is simple, it has low yield and is sonic treatment to obtain layered BN NSs [194]. However, ultra
only suitable for laboratory synthesis. LPE is considered to be an sonication in liquid can cause defects or rupture of NSs. Comparatively,
important method for large-scale production of phosphorene NSs [188]. CVD method can produce high-quality BN nanolayers over a large area
The BP bulk were uniformly dispersed in specific solvents (such as NMP, [195].
DMA, N-cyclohexyl-2-pyrrolidone, etc.), and then ultrasonication,
shearing, and centrifugation were carried out to further obtain a few
14
Fig. 8. (a) Formation process of the MoS2/VS2 heterostructure [174]. Reproduced with permission from ref. 174. Copyright 2020, WILEY-VCH.; (b) Schematic
diagram of MoTe2 transistor, (c) Dynamic sensing performance toward NO2 in N2 environment at concentration from 20 ppb to 2 ppm under different light illu
mination. Inset: dynamic sensing behaviors to NO2 at concentration from 20 to 200 ppb [176]. Reproduced with permission from ref. 176. Copyright 2018, American
Chemical Society.; (d) RT sensing responses of BP flakes to H2 (black curve), NH3 (blue curve) and NO2 (red curve) [193]. Reproduced with permission from ref. 193.
Copyright 2016, IOP Publishing Ltd.; (e) Summary of gas response of the pristine BP, Au/BP and Pt/BP for various target chemical analytes, (f) Gas response of Pt/BP
and pristine BP toward various H2 concentrations [195]. Reproduced with permission from ref. 195. Copyright 2017, American Chemical Society.; (g) Transient
response of 2D mesoporous g-C3N4 NSs towards varying concentrations of ethanol from 0.5 to 50 ppm at 303 K, (h) Respons and recovery times of mesoporous g-C3N4
NSs towards 50 ppm of ethanol at RT [199]. (i) Flowchart for the preparation of α-Fe2O3/g-C3N4, (j) The responses of the pure g-C3N4, α-Fe2O3, and α-Fe2O3/g-C3N4
(CF-0.6) versus different ethanol concentrations operating at 340 ◦ C [200]. Reproduced with permission from ref. 199. Copyright 2021, Elsevier.; ref. 200. Copyright
2016, Elsevier.; (k) Response under exposure to toluene, benzene, ethanol, methanol, and acetone at 140 ppm [205]. Reproduced with permission from ref. 205.
Copyright 2020, American Chemical Society.; (l) Sensor response to different gases at 200 ◦ C for Mg-MOFs gas sensors [211]. Reproduced with permission from ref.
211. Copyright 2019, Multidisciplinary Digital Publishing Institute.; (m) Sensor response (left) and recovery (right) shown in close up for 15,000 ppm propane
exposure [214]. Reproduced with permission from ref. 214. Copyright 2016, WILEY-VCH. (For interpretation of the references to colour in this figure legend, the
reader is referred to the Web version of this article.)
2.3.2. Research status of other 2DMs gas sensors Phosphorene is a single layer puckered honeycomb structure of BP,
which has a limited bandgap and high carrier mobility [37]. These
(1) BP-based gas sensors characteristics make phosphorene a promising gas sensing material. As
early as 2014, Chen’s team used first principles to investigate adsorption
15
of gas (such as carbon oxide and nitrogen oxide) on the monolayers of properties [43]. Yu et al. studied the adsorption behaviors of different
phosphorene, and determined the adsorption location of these gas gas (such as NH3, H2, CH4, etc.) on monolayer MXenes NSs by using first
molecules on the phosphorene [196]. Yang et al. studied the adsorption principles simulation. The calculated results demonstrated that only
behaviour of phosphorene on SO2 and H2S [197]. The results show that NH3 can be chemisorbed by MXenes NSs with high sensitivity [207]. In
SO2 is more easily adsorbed on phosphorene and has higher electron addition, Lee et al. reported the gas sensitive properties of Ti3C2TX gas
transfer. In addition, Donarelli et al. fabricated BP-based gas sensor, sensors for ethanol, methanol, acetone and NH3 at RT (25 ◦ C). The test
which was casted BP flakes by chemical exfoliation method on silicon results show that Ti3C2TX sensor has also the highest response (0.21) to
Si3N4 substrates with Pt interdigitated electrodes [198]. As described in 100 ppm NH3, while the response to 100 ppm of other VOCs is lower
Fig. 8d, this BP sensor has no response to CO and CO2 at RT, and has a (0.115 for ethanol, 0.143 for methanol, 0.075 for acetone) [208].
small but stable sensitivity to H2. The detection limits for NO2 and NH3 Exhilaratingly, a high sensitivity Ti3C2TX VOCs sensor appeared, which
are 20 ppb and 10 ppm. In same year, a research team led by professor has a low detection limit of 50 ppb for VOCs gases at RT [209]. Recently,
Cho studied the comparison of sensing performance of BP sensor, MoS2 Guo and co-workers prepared a novel Mo2CTX MXene gas sensor on a
sensor and graphene sensor at RT for NO2 with 0.1–100 ppm [199]. The silicon/silica substrate to detect VOCs. As shown in Fig. 8k, Mo2CTX
research results established that BP sensor to 1 ppm NO2 has higher MXene gas sensor has a higher selectivity to toluene. The response to
response value (80%), which is 20 times higher than MoS2 sensor and 140 ppm toluene is 2.81, and the response value to benzene, ethanol,
graphene sensor, and the detection speed is about 40 times faster. This is methanol and acetone are 0.97, 0.73, 0.58 and 0.14%, respectively
because the BP sensor has higher adsorption energy for NO2. This result [210].
directly confirms the prediction of Chen et al.
Using noble metals to functionalize the surface of BP can further (4) MOFs-based gas sensors
improve gas sensing performance of BP sensors. Subsequently, the effect
of noble metal (Pt) functionalization on gas sensing performance of BP MOFs are porous nanocomposites in crystalline form that are self-
sensors was interpreted [200]. The pristine BP sensor can only detect assembled from inorganic metallic node molecules with organic li
paramagnetic molecules such as NO2 and NO (which have a high gands [211]. Chemical sensors are highly dependent on surface re
response to NO2), but have little response to VOCs. Nonetheless, after actions. MOFs with large surface area and ultra-high porosity are widely
adding Pt, the Pt/BP sensor can detect low concentration of H2 and have used in gas sensing. The existence of metal and functional groups in
a higher response value (Fig. 8e). Fig. 8f presented the gas responses of MOFs can be coupled with gas molecules through hydrogen bonds, van
the original BP sensor and the Pt/BP sensor to different concentrations of der Waals interactions, and electrostatic interactions, resulting in su
H2 (10–10000 ppm). It is obvious that the Pt/BP gas sensor is highly perior gas sensing properties [212]. In 2015, the group of Dinca reported
sensitive and selective to H2. Apart from this, the Pt functionalized BP 2D MOFs based gas sensors for the first time [213], and this sensor
nanocomposites were prepared using a one-step reduction method by detected sub-ppm levels of NH3 at RT, and with a minimum detection
Liang et al. to detect NOx gas molecules [201]. The experimental results limit of 0.5 ppm. In the same year, this group constructed a
show that the response value of Pt functionalized BP hybrids to 10 ppm cross-reaction sensor array using 2D MOFs that allowed for a clear
NOx in a short time of 1.93 s is 2.19, and greatly improves the sensing distinction between different classes of VOCs [214]. The 2D MOFs array
performance of BP sensor. In addition, Lei et al. studied the effect of has a high response to polar VOCs and a low response to aliphatic hy
other noble metals (Li, Na, K, etc.) functionalization on gas sensing drocarbons. In addition to pure MOFs-based gas sensors, metal and
properties of phosphorene sensors by first principles calculations [202]. metal oxide NPs combined with MOFs have also been tried for appli
The results demonstrate that the presence of these metals can improve cation in gas sensing [215]. Lee et al. studied the gas-sensitive perfor
the adsorption of CO on phosphorene. mance of novel Mg-incorporated MOFs gas sensors [216]. As shown in
Fig. 8l, Mg-MOFs gas sensor has good selectivity and sensing response to
(2) g-C3N4-based gas sensors 50 ppm NO2 (response value is about 1.33). In addition, the Mg-MOFs
gas sensor has a short response and recovery time to 10 ppm NO2
Due to its inherent porous structure and lone pair electrons on N (167 s and 92 s, respectively). In 2020, Ma et al. successfully prepared
atoms in g-C3N4, it has been widely used in RT gas sensor. At first, Wang In2O3 porous hollow rod (PHRs) gas sensors using MOFs as a template
et al. reported a g-C3N4 gas sensor, which can detect 140 ppb NO2 at RT [217]. The experimental results show that the In2O3 PHRs gas sensor has
(under 65% RH) [203]. The super gas sensing properties are associated a high sensitivity and selectivity to 10 ppm Cl2 at 160 ◦ C. Moreover, the
with the good binding affinity between rich pyridine N atoms and NO2 In2O3 PHRs gas sensor has a low detection limit (3.2 ppb).
molecules. The synthesis of g-C3N4 composite materials is an efficient
way to improve gas sensing performance. Recently, Srinivasan et al. (5) BN-based gas sensors
studied the ethanol sensitive performances of g-C3N4 gas sensor at RT
[204]. As shown in Fig. 8g and h, the response of g-C3N4 sensor to 50 In 2013, Feng et al. prepared BN NSs by short-pulse-laser-produced
ppm ethanol vapor is 182.4. The minimum detection limit at RT is 500 plasma deposition technique and applied them to detect CH4 and O2
ppb. Furthermore, the formation of heterojunction between g-C3N4 and [218]. The experimental results show that the response value of the
metal oxide can improve gas sensitivity. Zhang and his colleagues utilize BN-based gas sensor at 150 ◦ C to 100 ppm CH4 is 780%, the response
hydrothermal method to develop α-Fe2O3/g-C3N4 ethanol sensor time and recover time are 10 s and 15 s, respectively. Compared with O2,
(Fig. 8i) [205]. The α-Fe2O3/g-C3N4 gas sensor shows better gas sensi the BN-based gas sensor has better sensitivity to CH4. In addition, atomic
tivity than g-C3N4 gas sensor due to the formation of heterojunction doping can improve the performance of BN gas sensors. Maboudian et al.
(Fig. 8j). Guo et al. grew highly ordered Ni-doped SnO2 NSs on g-C3N4 prepared a Pt-BN aerogel gas sensor to detect propane. Compared with
films by calcination and hydrothermal methods, and successfully pre BN-based gas sensor, the response of Pt-BN to propane is faster, and the
pared Ni–SnO2/g-C3N4 to detect acetone [206]. The results showed that response and recover time of Pt-BN to 1500 ppm propane are 1.35 s and
the response of Ni–SnO2/g-C3N4 to 10 ppm acetone was about 142.5, 0.6 s (Fig. 8m) [219].
and its detection limit was as low as 1.38 ppb.
2.3.3. Problems of other 2DMs gas sensors
(3) MXenes-based gas sensors Surface functionalization [220] and vertical array structure [146]
are available to widely improve the sensitivity of 2DMs gas sensors.
MXenes have shown great potential in gas sensing owing to high However, 2DMs gas sensors have several limitations such as poor
electrical and thermal conductivity, tunable electronic and chemical response [179], long time to recover, slow gas molecular desorption at
16
RT [180]. Over a long period of time, the surface of 2DMs will be (Fig. 9).
partially covered by O2 or water in air, gradually reducing the sensing
performance and long-term stability [221]. So, we still need to delve 3.1. Design and preparation of 2DMs
into more methods to improve gas sensitive performance of 2DMs gas
sensors. Some researchers provide some strategies (such as light-assisted 3.1.1. Regulation of microstructure
enhancement of gas sensing property) improve sensing properties [222, The sensing material is one of the most critical parameters to
223]. For example, the irradiation of UV will generate more conductive determine the sensing performances. In the process of chemical syn
electrons and promote the electron transfer under UV irradiation, thus thesis, NSs of 2DMs tend to agglomerate and stack. This makes it difficult
improving the gas response [224]. to identify the type and concentration of defects, the position of con
duction band and valence band, and even the size and number of layers
3. Conclusions and perspectives of 2DMs are difficult to control. The conductivity and semiconductor
properties of 2DMs are difficult to reflect. The number of gas adsorption
In recent years, 2DMs have been widely used in gas sensing with and reaction sites on the surface of 2DMs is insufficient. Although the
respect to their unique structure and physical and chemical properties methods of heteroatom doping and heterostructure construction can
(high conductivity, large specific surface area, etc.). In this paper, the effectively improve gas sensing performance [225–228], individual
research progress of some common 2DMs (such as graphene, TMDs, BP, structural, physical and chemical properties have not been fully utilized.
g-C3N4, Mxenes, etc.) used in gas sensors is reviewed. 2DMs can also It is very necessary to develop more sophisticated nanoscale processing
detect the target gas at RT. However, due to the lack of defects on the methods to regulate microstructure and morphology of 2DMs (such as
surface, adsorption of oxygen, and the difficulty in regulating the band size, pore defect etc.) [229–231], improve the dispersion of 2DMs in
gap, the gas sensors based on graphene and other 2DMs have poor solvents and stability in air, such as ion beam sputtering, electro
sensitivity characteristics, showing slow response and incomplete re chemical synthesis, inkjet printing, laser processing, 3D printing, etc. In
covery at RT. Although the response and recovery characteristics can be addition, it is possible to identify defect and morphology structure by
enhanced through chemical modification, doping modification and theoretical calculation method, understand the key parameters and
other strategies to improve the sensitivity of the sensor, but compared formation mechanism of defect formation, and develop effective
with traditional metal oxide sensor sensitivity characteristics still lag. methods and technologies for preparing and controlling defects.
Therefore, it is very important to propose some effective strategies to
develop high performance 2DMs based gas sensors in our future works
Fig. 9. Schematic diagram of challenge and effective approach of development high performance gas sensor. Reproduced with permission from ref. 217. Copyright
2018, American Chemical Society.; ref. 218. Copyright 2019, American Chemical Society.; ref. 220. Copyright 2018, American Chemical Society.; ref. 221. Copyright
2018, American Chemical Society.; Reproduced with permission from ref. 222. Copyright 2021, Elsevier.; Reproduced with permission from ref. 223. Copyright
2020, American Chemical Society.; Reproduced with permission from ref. 224. Copyright 2020, Elsevier.; Reproduced with permission from ref. 225. Copyright
2016, American Chemical Society.; ref. 226. Copyright 2018, American Chemical Society.; Reproduced with permission from ref. 227. Copyright 2021, Elsevier.;
Reproduced with permission from ref. 228. Copyright 2015, Springer Nature.; Reproduced with permission from ref. 229. Copyright 2017, Springer Singapore.;
Reproduced with permission from ref. 230. Copyright 2018, Elsevier.; Reproduced with permission from ref. 231. Copyright 2015, American Chemical Society.;
Reproduced with permission from ref. 232. Copyright 2021, WILEY-VCH.; Reproduced with permission from ref. 233. Copyright 2021, Elsevier.; ref. 234. Copyright
2019, Elsevier.
17
3.1.2. Contact between 2DMs and substrate equipment, achieving zero power consumption, energy saving and
Generally, the sensing materials need to be deposited onto the sur environmental protection. The nanoactuators transform the mechanical
face of by diverse processing techniques (such as traditional drip energy around the sensor into electrical energy. By adjusting the
coating, rotary coating and steam plating methods). As a result, the polarizing electric field at the interface and surface, high-performance
sensing film is inhomogeneous and high interfacial resistance exists sensing and energy storage can be obtained, providing self-powered
between the sensitive film and the contact electrode. The stability and characteristics. Researchers at home and abroad have carried out
repeatability of sensor is reduced. The high interface resistance leads to abundant research on the integrated design and synergistic effect of
the increase of sensor resistance, the small current value of the test nanomaterials actuators and gas sensitive devices [240].
circuit, and the test signal is susceptible to external interference. Hence, Wearable sensors combine with wireless technology are integrated to
it is an effective method to improve the stability and repeatability of an end-user with the Internet of Things and offer real-time information.
sensor to study the reliable preparation technology of sensitive film. In The gas sensing data need to be transmitted either to phone, computer
general, the uniform sensitive films are prepared by physical/chemical and the cloud server for analyzing and visualizing. It is portable to
vapor deposition, magnetron sputtering, photolithography and other receive sensing data from a distance. At present, wireless transmission
methods. However, these processes need to be implemented under harsh technologies, including near field communication (NFC), infrared
conditions such as high temperature and vacuum. The sensing materials communication technology, radio frequency identification (RFID),
and substrate can be directly integrated, which is good choice for the wireless fidelity (Wi-Fi), Bluetooth, ZigBee and others, have been
fabrication of high-quality sensors. For example, the sensor with stable available to wirelessly transmit gas sensing data to terminal. In view of
structure is prepared by in-situ assembly membrane technology, pre- monitoring gas sensors wirelessly, the presence of transmission tech
wetting the substrate surface and forming uniform sensitive film spon nology should be upgraded result from the requirement of small size,
taneously on the substrate surface through chemical bonding. Therefore, low power, integrated circuit design, and difficulty of low transmission
further development of effective strategies to improve the contact be rate and weak anti-interference ability.
tween 2DMs and substrate is very necessary.
3.3. Gas sensing mechanism
3.2. Fabrication of gas sensors
3.3.1. Theoretical calculation and in-situ characterization
3.2.1. MEMS based gas sensors and gas sensor arrays The gas adsorption process on the surface of sensitive materials in
In generally, 2DMs can also be used as the sensing materials for volves complex physical and chemical processes such as surface chem
miniaturized, portable and low-power MEMS based gas sensors. These ical reaction, carrier transport, utilization efficiency of sensitive
sensors are fabricated on silicon-wafer by using micro/nano manufac materials and others. In fact, the low gas sensitivity of 2DMs is closely
ture technologies [231–233]. However, several key issues, such as connected with ill-defined gas sensing mechanism. For the sake of
process compatibility with microelectronics due to some explaining gas sensing mechanism, DFT, computational modeling,
high-temperature processing and reliable assembly procedures to analysis of microstructure-sensing property relationships via in-situ
assemble the ideal nanostructures with silicon-based platforms. As a characterization is required [229,241–243]. Gas selectivity can be
matter of fact, the monitoring of the pollutant gases in the environment studied by calculating adsorption energy, charge transfer and energy
can not be depend on only one certain gas. It is very meaningful to state density. These research methods provide a theoretical basis for the
develop gas sensor arrays that can obtain the discrimination of different construction of high-performance gas sensors. Through the above
gases. Besides, sensor arrays with the assistant of a smart algorithm, for research, it is found that the research on gas sensitivity mechanism has
example principal components analysis (PCA), machine learning and not formed a complete theoretical system.
other analysis methods, are promising in accurately detecting and
discriminating coexisting gases and play a major role in the fields of 3.3.2. Influence of humidity on gas sensitivity
harmful gas monitoring, non-traumatic disease marker, food safety, etc. The humidity in the environment affection the performance of the
sensor sensitivity cannot be ignored [244], the surface of materials
3.2.2. Flexible and wearable gas sensors usually has strong moisture absorption. Water molecular and oxygen to
Recently, with the development of flexible and wearable E-skins, form the competition effect, the adsorption of H2O leads to the material
2DMs and flexible substrate have potential in gas sensors [234–236]. surface oxygen adsorption capacity and adsorption gas of the decrease in
Flexible gas sensors with low weight, good flexibility, excellent the number of active site, leading to significantly lower the sensitivity of
stretchability and outstanding conformability have significance in the sensor [243,245]. We have studied the gas-sensitive characteristics
monitoring gaseous pollutants, VOCs, humidity, exhaled gas marker, of Zn2SnO4-RGO to NO2 under different humidity conditions [246], and
gases released by food at RT [237–239]. Although many approaches found that Zn2SnO4-RGO had the highest sensitivity to NO2 under 80%
have been used in fabricating flexible and wearable gas sensors, inte RH condition, and characterized by in-situ diffusion infrared spectros
grated and multifunctional wearable gas sensors need to be further copy (DRIFT). In-depth study on the chemical reaction and charge
identified various gases in a complex atmosphere. In order to adapt to transfer of NO2 and H2O molecules on the surface of the material in the
the trend of sensor wearability, the sensing material should be process of NO2 sensing.
biocompatible, nontoxic and self-healing to attach to the surface of In this review, we summarized the research status and challenge of
human skin. Apart from this, sensitivity and reproducibility of flexible RT chemiresistor gas sensors based on 2DMs. The advantages of various
gas sensor needs to be greatly improved in the absence of heating and 2DMs and their gas sensing applications were clearly elucidated. Finally,
light irradiation. we discussed the development and challenge from three aspects: design
and preparation of 2DMs, fabrication of gas sensors and gas sensing
3.2.3. Smart self-power and wireless gas sensors mechanism. We believe that the development of gas sensing technology
Power plays a dominant part in receiving and transmitting sensing based on 2DMs is very desirable and diverse, thanks to their unique
signals during gas sensing process. The bulky power supplies and wired physical and chemical properties. The development trend of gas sensor
data transmission system, which further limits their applicability in real- is miniaturization, networking, intelligent, modular to advance quality
life condition. Besides, the wearable devices with battery-powered of life.
require replacement. Self-power technology is a new power supply
technology. It converts all kinds of energy in the surrounding environ
ment into electric energy to drive the operation of low-power electronic
18
Declaration of competing interest ALD atomic layer deposition

HA-MoS2 horizontally aligned MoS2
The authors declare that they have no known competing financial MHVA-MoS2 mixture of horizontally and vertically aligned MoS2
interests or personal relationships that could have appeared to influence VA-MoS2 vertically aligned MoS2
the work reported in this paper. FEM finite element method
QDs quantum dots
Data availability AA-CVD aerosol-assisted CVD
PB purple blue
Data will be made available on request. LET liquid exfoliation technique
RP red phosphorus
Acknowledgements LB langmuir-blodgett
PHRs porous hollow rod
This work was supported by National Natural Science Foundation of PCA principal components analysis
China (Grant No. 52104189, 11632004 and U1864208), Natural Science NFC near field communication
Foundation of Hebei Province (F2020202050), National Science and RFID radio frequency identification
Technology Major Project (2017-VII-0011-0106), Science and Tech Wi-Fi wireless fidelity
nology Planning Project of Tianjin (20ZYJDJC00030), the Key Program DRIFT diffusion infrared spectroscopy
of Research and Development of Hebei Province (202030507040009),
the Fund for Innovative Research Groups of Natural Science Foundation References
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Composites Part B 248 (2023) 110378

Contents lists available at ScienceDirect

An overview on room-temperature chemiresistor gas sensors based on 2D

1. Introduction semiconductor, electrochemical, solid electrolyte and contact combus

1.1.1. The sensing mechanism of semiconductor resistive gas sensors

1.1.2. The challenge of semiconductor resistive gas sensors

Pd-RGO NO2 25 ~1.65 − /− 25 [76]

SnO2-RGO NO2 5 ~3.31 − /− 1 [81]

MoS2 NO2 500 ~300% 180/480 25 [120]

BP NO2 1 ~80% ~70/- 0.1 [194]

Declaration of competing interest ALD atomic layer deposition

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1-s2.0-S135983682200751X-main

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1-s2.0-S135983682200751X-main

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1-s2.0-S135983682200751X-main

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Composites Part B 248 (2023) 110378

Contents lists available at ScienceDirect

An overview on room-temperature chemiresistor gas sensors based on 2D

1. Introduction semiconductor, electrochemical, solid electrolyte and contact combus­

1.1.1. The sensing mechanism of semiconductor resistive gas sensors

1.1.2. The challenge of semiconductor resistive gas sensors

Pd-RGO NO2 25 ~1.65 − /− 25 [76]

SnO2-RGO NO2 5 ~3.31 − /− 1 [81]

MoS2 NO2 500 ~300% 180/480 25 [120]

BP NO2 1 ~80% ~70/- 0.1 [194]

Declaration of competing interest ALD atomic layer deposition

You might also like

1. Introduction semiconductor, electrochemical, solid electrolyte and contact combus