1 s2.0 S2211285520309460 Main

Nano Energy 79 (2021) 105369
Contents lists available at ScienceDirect
Nano Energy
journal homepage: http://www.elsevier.com/locate/nanoen
Recent advances in energy-saving chemiresistive gas sensors: A review

Sanjit Manohar Majhi a, b, 1, Ali Mirzaei c, 1, Hyoun Woo Kim a, b, **, Sang Sub Kim d, ***,
Tae Whan Kim e, *
a
Division of Materials Science and Engineering, Hanyang University, Seoul, 04763, South Korea
b
The Research Institute of Industrial Science, Hanyang University, Seoul, 04763, South Korea
c
Department of Materials Science and Engineering, Shiraz University of Technology, Shiraz, 715557-13876, Iran
d
Department of Materials Science and Engineering, Inha University, Incheon, 22212, South Korea
e
Department of Electronics and Computer Engineering, Hanyang University, Seoul, 04763, South Korea
A R T I C L E I N F O A B S T R A C T
Keywords: With the tremendous advances in technology, gas-sensing devices are being popularly used in many distinct
Energy saving areas, including indoor environments, industries, aviation, and detectors for various toxic domestic gases and
Low-power consumption vapors. Even though the most popular type of gas sensor, namely, resistive-based gas sensors, have many ad
Room-temperature sensing
vantages over other types of gas sensors, their high working temperatures lead to high energy consumption,
MEMS-Based gas sensors
Flexible gas sensors
thereby limiting their practical applications, especially in mobile and portable devices. As possible ways to deal
with the high-power consumption of resistance-based sensors, different strategies such as self-heating, MEMS
technology, and room-temperature operation using especial morphologies, have been introduced in recent years.
In this review, we discuss different types of energy-saving chemisresitive gas sensors including self-heated gas
sensors, MEMS based gas sensors, room temperature operated flexible/wearable sensor and their application in
the fields of environmental monitoring. At the end, the review will be concluded by providing a summary,
challenges, recent trends, and future perspectives.
1. Introduction composition and damage to the lungs, making humans more vulnerable
to diseases such as COVID-19 [7]. Accordingly, air pollution has become
Due to rapid industrialization and urbanization, the world is facing a pressing global problem, prompting several health agencies to
the problem of severe air pollution, as witnessed by the increasingly recommend short-time exposure limits (STELs) for various toxic and
large amounts of deleterious and pollutant gases being introduced into VOC gases [8,9]. Moreover, if the potential risk to human health is to be
the environment. To name a few, these pollutants consist of several toxic reduced, pollutant gases in the air must be continuously monitored using
gases such as CO, SO2, NO2 and H2S and/or chemicals and volatile sensitive and reliable electronic devices.
organic compounds (VOCs) such as benzene, toluene, ethanol, acetal Nowadays, the detection of dangerous gases is becoming increas
dehyde and formaldehyde. The presence of toxic gases and VOCs can be ingly important in different industries, indoor and outdoor air quality
detrimental to humans and the surrounding atmosphere [1–3]. For monitoring, public safety, mines, and so on [8–11], As a result,
instance, an estimated 3.8 million people per year face severe illnesses numerous sensing techniques, such as the electrochemical [12], optical
that may prove fatal and can be attributed to air pollution. Moreover, fiber [13], quartz crystal microbalance (QCM) [14] and capacitive [15]
near 20% of cardiovascular deaths and about 20% of deaths due to techniques, have been applied for this purpose. However, most of these
stroke can be attributed to household pollution [4]. Moreover, toxic techniques have disadvantages such as relatively high price, low sensi
gases can significantly affect the respiratory tract and may even be tivity and selectivity, sophisticated design, and a need for additional
harmful to the nervous and the immune systems [5,6]. In particular, equipment; some even lack portability [16]. Among them, metal oxide
severe air pollution can cause abnormalities in lung surfactant semiconductor (MOS) gas sensors, working on the basis of changes in
* Corresponding author.
** Corresponding author. Division of Materials Science and Engineering, Hanyang University, Seoul, 04763, South Korea.
*** Corresponding author.
E-mail addresses: [email protected] (H.W. Kim), [email protected] (S.S. Kim), [email protected] (T.W. Kim).
1
Equal contribution.
https://doi.org/10.1016/j.nanoen.2020.105369
Received 13 July 2020; Received in revised form 3 September 2020; Accepted 7 September 2020
Available online 17 September 2020
2211-2855/© 2020 Elsevier Ltd. All rights reserved.
S.M. Majhi et al. Nano Energy 79 (2021) 105369
Fig. 1. Schematic illustration of the basic sensing principle for (a) n- and (b) p-type MOS gas sensors. Reprinted from Ref. [29] with permission from Elsevier
(Copyright 2020).
resistance in the presence of a target gases, have attracted great atten (Fig. 2(b)), which changes the conductivity, and thus the resistance, of
tion and have become a hot research topic [17] because of their the gas sensor [26–28].
numerous and unique characteristics, such as high sensitivity, short Traditionally, chemiresistive-based sensors consist of three compo
response/recovery time, ease of fabrication, high stability, simple nents: namely, the insulating substrate (typically alumina or silicon
operation and low price [18,19]. oxide), interdigitated electrodes, and a heater under the substrate to
The modulation of the electrical resistance or conductance in a target heat the sensor [31]. Generally, MOS-based gas sensors work at high
gas environment is known to be the basic gas sensing mechanism of a temperatures (100–450 ◦ C) [32]; however, this heating process results
resistive-based sensor [20,21]. Initially in air, upon adsorption of oxy in some issues, such as degradation of the long-term stability due to the
gen molecules, an electron depletion layer (EDL) for n-type materials aggregation and coarsening of nanograins, an increase in fabrication
and a hole accumulation layer (HAL) for p-type materials will be formed cost due to the addition of the heater and high power consumption (100
on the sensor’s surface. When an n-type MOS is exposed to an oxidizing mW up to 1 W) [33–36]. In this regard, power consumption is a chal
gas, its resistance increases while for reducing gases the resistance de lenging issue that limits the integration of MOS-based gas sensors into
creases [22]. Fig. 1(a)-(b) schematically show the principle underlying some important portable devices.
the gas sensing mechanism of n- and p-type MOS-based resistive gas Due to the advances in smart phone technology, various sensors are
sensors [23]. now being integrated into cell phones for various applications, such as
The typical sensing mechanisms can be described by using the band healthcare, public safety, and environmental and food monitoring [37].
bending theory. MOS materials are known to have many nanograins of The current chemiresistive sensors are not suitable for battery or
different sizes and electrons are believed to flow in the grain boundaries. portable operation due to the high temperatures needed for operation.
After oxygen gas molecules have been adsorbed on the sensor’s surface, Thus, the design of portable, low-cost and low power consuming or
an electron will be extracted from the conduction band (CB), and an EDL energy-saving gas sensors is essential for their use in wireless and
will be formed in n-type MOS gas sensors [24]. This process results in portable devices [38,39]. Thus, many attempts, such as the uses of
energy-band bending as shown in Fig. 2(a). Due to presence of grains, low-power light-emitting diodes (LEDs) [40], noble-metal functionali
Schottky barriers with a height of V1 will be initially formed in air, as zation [41] and hybrid materials [42], have been made to lower the
shown in Fig. 2(b) [25]. The reaction of oxygen ionic species with energy consumption of gas sensors by decreasing the optimum sensing
reacted gases can change the height of the Schottky barrier to (V2) temperature. Moreover, two other promising techniques to reduce
2
Fig. 2. (a) Schematic of the resistance change of an n-type MOS gas sensor during reducing gas (H2) detection, (b) surface charge layer model, and (c) grain boundary
barrier model. Reproduced from the Ref. [30] under the Creative Commons attribution 4.0 License (CC BY 4.0/). Copyright 2020, IOP Science.
power consumption significantly are operation of gas sensor in a this article, we will focus mainly on a special category of self-powered
self-heating mode [43] and integration of gas sensors into MEMS plat gas sensors, namely, self-heated gas sensors.
forms [44].
In this review article, we have discussed the current advancements of 2.1. Self-heated gas sensors
energy-saving gas sensors based on chemiresistive principle (Fig. 3).
This review article discusses several topics: self-heated gas sensors, low- As discussed, the energy consumption must be lowered if battery-
power MEMS-based gas sensors, and gas sensors operating at room operated gas-sensing devices are to be designed. In practice, for the
temperature with their applications including flexible/wearable gas gas sensors used in mobile or wireless network devices power con
sensors, and their associated gas sensing mechanisms. At the end, the sumption is in the range of several microwatts [27]. Typically, a con
review is concluded with brief summary and future perspectives on the ventional thick or thin film gas sensor equipped with a heater consumes
possible opportunities for further developing energy-saving gas sensors. about 1–5 W during its operation (Fig. 4(a)). On the other hand,
MEMS-based gas sensors consume less than 30–50 mW to reach tem
2. Self-powered gas sensors peratures up to 500 ◦ C. Also, for a self-heated gas sensor without an
external heater, much less power is consumed [61]. The main factors
Piezoelectric nanogenerators (PENGs) and triboelectric nano underlying self-heating gas sensors are the application of an appropriate
generators (TENGs) enabling the monitoring of gases at RT in a self- voltage, with Joule heating generating heat inside the sensor, thereby
powered way have been introduced by Zhong Lin Wang’s group increasing its temperature. As shown schematically in Fig. 4(b), in this
[45–47] In regard to PENG-based gas sensors, pure ZnO has been mode of operation, an external voltage is directly applied to the sensor
investigated, with the piezoelectric output being generated by ZnO electrodes. Nevertheless, for self-heated gas sensors, realization of high
acting as both a gas sensing signal and power supply [48,49]. Also, sensitivity at an appropriate bias voltage still remains a challenge [62].
several metals, such as Cu [50], Pd [51], Au [52], and Pt [53], have been The efficient self-heating (ESH) coefficient for a self-heated gas
incorporated in order to enhance the catalytic reactions and, thus, the sensor can be expressed as
sensing performances. In addition, due to the many benefits, including
increased modulation of the resistance, of ZnO-comprising hetero ESH = ΔT/Q (1)
structures, including ZnO/SnO2 [54], ZnO/NiO [55], and ZnO/In2O3
[56], they have been employed to enhance the sensing capabilities, where ΔT is the temperature increase due to the applied voltage, and Q
providing excellent performances, owing to their stronger output signal is the electrical power dissipation. Typically, an ESH value greater than
[47]. TENGs can be used to monitor gases because the surface adsorbed 1 (ESH > 1) is beneficial for self-heating, which means an increase of a
species strongly affect the effectiveness of triboelectric charging [57]. few Kelvin/microwatt consumed. Conventional self-heating sensors (ΔT
The first TENG-based gas sensor was comprised of polymer films such as ~ 500 ◦ C and P ~ 10 mW) have ESH values of ~ 0.05 [63]. In general,
polyamide (PA) and polytetrafluoroethylene (PTFE) [57]. Subsequently, MOS materials with nanowire (NW) morphology are preferred for
a variety of materials, such as ZnO [58], polyaniline (PANI) [59], and self-heating studies [63]. As the NWs serve as pathways for electron
poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) transfer, the lengths of the NWs directly affect the heat generated inside
[60], has been adopted. Because we are dealing with the gas sensor, thereby allowing Joule heating to warm effectively the
chemiresistive-based gas sensors and the number of pages is limited, in NWs and ensuring a higher response to the target gas. Furthermore,
power is consumed at microwatt levels owing to the minimal thermal
3
Fig. 3. An overview of the main techniques and applications of the energy-saving gas sensors discussed in this review paper.
capacitance of the NWs [32,65,66]. Moreover, the diameter of the NW is exhibited an enhanced response (Rg/Ra = 4.6) towards NO2 at 20 ppm.
important because the temperature increase has an indirect relation The sensing mechanism was explained based on modifications of the
with the radius of the NW; thinner NWs produce larger increases in the potential barriers at the SnO2 NW-NW junctions and establishment of
temperature [63]. depletion layers at the SnO2 NWs [75]. When the sensors were exposed
In 2003 and 2006, Salehi et al. and Lee at al. introduced self-heated to NO2 gas, NO2 molecules were adsorbed on the surface of the SnO2 NW
gas sensors based on SnO2 and NiO thin films for the detection of CO and sensor, and electrons were extracted from the conduction band of SnO2
formaldehyde, respectively [64,65]. These systems showed lower power NWs to form NO−2 ionic species [76], which resulted in an increased
consumption as compared to conventional gas sensors. For further de number of depletion layers and potential barriers with increased
creases in the energy consumption of the MOS gas sensors, NW mor heights.
phologies are preferred due to the aforementioned advantages. The first The reduction of power consumption in the self-heated sensors de
NW-based self-heated sensor was introduced by Strelcov et al. [67], and pends on the sensing area of the electrode, and the design of head-to-
so far, the self-heating properties of single NW [66,68–70], multiple head electrodes is an important aspect that is often neglected. Ngoc
NWs [67,68,71] and networked NWs [61,68] have been reported. As et al. introduced a self-heated NW gas sensor based on SnO2 NWs grown
compared to the single-NW and the network-type NW sensors synthe using a chemical vapor deposition (CVD) technique, in which SnO2 NW
sized by using off-chip methods, on-chip NW sensors have many ad networks bridged the electrode gaps [63]. They investigated the effect of
vantages [43,63,72,73]. Therefore, on-chip networked NW gas sensors the electrode gap size on the sensing performance. For that purpose, the
are being developed for self-heating purposes; in this context, the head-to-head electrodes gaps were maintained at 2, 5, 10 and 20 μm,
on-chip methods are used to obtain power consumption at μW level [61, which were labelled as G2, G5, G10 and G20, respectively. The mean
67]. Hieu and co-workers reported the synthesis of on-chip grown net diameter of the fabricated SnO2 NWs was 80 nm. The electrode with a
worked SnO2 NWs [74]. Prior to the on-chip growth, the electrode was small gap was seen to yield a dense SnO2 NW network (G2 with densest
designed using a photolithography method (Fig. 5(a)). After that, SnO2 nanojunction) whereas the electrode with a large gap filled with a sparse
NWs having average diameters around 95 nm were grown using a network (G20) had the sparsest nanojunction. The sensor with a 20-μm
well-known vapor-liquid-solid (VLS) method (Fig. 5(a)). The sensor electrode gap (G20) displayed a good response (3.75) toward C2H5OH
showed a response of 2.1–2.5 ppm NO2 gas with a power consumption of (250 ppm) at a 10-mW power supplied. One of the merits in designing
only 25 mW, along with good selectivity. The authors further addressed head-to-head electrodes is reduced power consumption because the
reducing the size of the electrodes with a gap width of 10 μm (Fig. 5(b)) self-heated sensor is dependent on the electrode area [74]. The nano
and growing SnO2 NWs on the electrode (Fig. 5(b-e)). The sensor junctions between the SnO2 NWs established the Schottky barriers, of
4
Fig. 4. Schematics of (a) a conventional MOS-based gas sensor and (b) a MOS-based gas sensor in the self-heating mode. Adapted from Ref. 62 with permission from
Elsevier (Copyright 2020).
which increase the resistance at the nanojunction (Rj) as compared to reaction between Ag2O and H2S while the recovery time increases
the resistance at the NWs. Thus, one can conclude that for a self-heated because a longer time is required to change a large amount of Ag2S back
NW sensor, warm-up at the junction in a nanoscale range is more to Ag2O [79–81].
important than network heating [67]. In addition to Ag catalysts, Pt, Pd, and Au NPs have also been used in
Noble metal decoration is a good strategy to enhance the gas sensing studies of self-heating gas sensors [82–87]. These noble metal NPs are
characteristics of MOS-based gas sensors, which is due to the sensitiza generally functionalized on the surface of the gas sensor by using various
tion effects of noble metals [77,78]. In this regards, the effect of approaches, such as UV-irradiation [88], γ-ray irradiation [89], and
self-heating and the density of the catalytic material were investigated in sputtering [90]. In a recent study of gas sensors operating in the
Ag-decorated SnO2 NW networks by Ngoc et al. [33]. SnO2 NWs were self-heating mode, Kim et al. used UV-irradiation and sputtering tech
synthesized using a thermal evaporation method, and Ag nanoparticles niques to deposit both Pd and Pt NPs on the on-chip grown ZnO NWs for
(NPs) were sputter deposited on the surfaces of SnO2 NWs for different a selective study of benzene and toluene gases [78]. Initially, the ZnO
durations of 10, 20, 40 and 80 s to control the density of Ag NPs; NWs were synthesized through a VLS method followed by ultraviolet
accordingly, the sensors were named ST10, ST20, ST40, and ST80, (UV) irradiation technique to deposit Pd NPs while the Pt NPs were
respectively. They used as H2S gas sensor in the self-heating mode under deposited by using a magnetron sputtering method, followed by an
different powers of 2–20 mW [33]. Among the four sensors, the ST80 annealing treatment (Fig. 6 A). Morphologies of the synthesized Pd/ZnO
sensor showed the highest response of 21.2 to 0.5 ppm to H2S gas at a NWs and Pt/ZnO NWs are shown in Fig. 6(B) and (C), respectively. For
low heating power of 2 mW with an acceptable response/recovery time self-heating mode, both 5 nm-Pt-ZnO NWs and 5s-Pd-ZnO NWS sensors
of 18/980 s. Ag NPs are known for their ability to selectively react with were studied with different applied voltages from 1 to 20 V. The
H2S at low concentrations at temperatures below 200 ◦ C [79]. However, Pt/Pd-ZnO NWs sensors showed high responses to toluene and benzene,
when the power reached 20 mW, the authors reported serious thermal respectively, among other reducing gases. The highest response of the 5
damage of the sensing material. When the sensor is exposed to H2S gas, nm-Pt/ZnO NW sensor operating in the self-heating mode to 50-ppm
Ag2O NPs react with H2S gas molecules as follows: toluene was 2.74 at RT under a 20-V applied voltage whereas the
highest response obtained for the Pd/ZnO NW sensor under the same
Ag2O + H2S → Ag2S + H2O (2) conditions towards benzene (50 ppm) was 2.20 (Fig. 6 D and E). Also,
which is an exothermic chemical reaction that can occur at low tem the power consumptions for the Pt- and Pd-ZnO NW gas sensors were
peratures. During the recovery period, the following reaction is found to be 208 and 139 μW at 5 V, respectively. The good selectivity
expected: toward benzene and toluene can be ascribed to the combination of
catalytic effects of both Pt and Pd NPs, respectively. For benzene, the
2Ag2S + 3O2 → 2Ag2O + 2SO2 (3) following reaction has been reported:
which is an endothermic chemical reaction occurring at high tempera C6 H6 (g)→C6 H6 (ads) (4)
tures. Under low heating power, the reaction in Eq. (2) is dominant and
converts Ag2O into Ag2S with a metallic nature, leading to a loss of the p- C6 H6 (ads) + 15O− → 6CO2 + 3H2 O + 15e− (5)
n junctions between Ag2O and SnO2 and decreased sensor resistance.
and for toluene, the following reaction was reported:
Under high heating powers, the reaction in Eq. (3) increases, but never
dominates the reaction in Eq. (2). Therefore, under lower heating C7 H8 (g)→C7 H8 (ads) (6)
powers, a higher gas response is observed. Also, with increasing Ag
catalytic density, the response time decreases due to the high rate of the C7 H8 (ads) + 18O− → 7CO2 + 4H2 O + 18e− . (7)
5
Fig. 5. (a) Schematic illustration of the fabrication of networked SnO2 NWs. (b–e) FE-SEM images of networked SnO2 NWs grown on the sensor substrate after
reducing the electrode size. Reproduced from Ref. 74 with permission from the American Chemical Society (Copyright 2020).
Accordingly, the higher response of the Pt/ZnO NW sensor to toluene and 20 V. Two possible locations of Joule heating were the ZnO grains
relative to the response of the Pd/ZnO NW sensor to benzene was related and the networked ZnO-ZnO homojunctions [92].
to the higher electron donating capacity of toluene. Schematic diagrams Other than the single components, binary/ternary structures or
of the sensing mechanisms underlying pristine and Pt/Pd-ZnO NW heterostructures with different noble metal catalysts have been used for
sensors are provided in Fig. 6(F). sensing studies due to the synergistic effect resulting from the combi
When a voltage is applied, heat is generated because the electrons nation of the MOS structure and a noble metal, which results in
lose kinetic energy when they collide with other electrons or other ob enhanced sensing reactions, surface activities and selectivities towards
stacles in their paths. The relation between Joule heating per volume specific gases [93,94] Kim et al. reported Au-decorated SnO2-ZnO
(W/m3) and the applied voltage can be expressed as follows [91]: core-shell NW-based sensors for the investigation of the CO gas-sensing
properties under self-heating [83]. The SnO2 NWs were synthesized
J=V2/ρL2 , (8) vertically on chip by using the typical VLS method (Fig. 7a–b) [82].
where ρ is the resistivity of the sensing layer, and L is its length. The Then, ultrafine Au NPs were deposited on the sensor’s surface by using
temperature increase due the self-heating effect was found to be 0, 1.6, the γ-ray radiolysis technique (Fig. 7c). The ZnO shell thickness was
12.9, 25.8, and 80 ◦ C, respectively, for applied voltages of 0, 1, 5, 10, varied from 10 to 80 nm by performing 50 to 500 cycles of atomic layer
6
Fig. 6. (A) Scheme illustrating the procedures for the fabrication of the sensor chip (Step-1) followed by the on-chip growth of ZnO NWs (Step-II), and Pd and Pt
functionalization on ZnO NWs (Step-III); (B, C) morphology of Pt and Pd-ZnO NWs; (D, E) response values obtained for Pt and Pd-ZnO NWs sensors with respect to
applied voltages; (F) toluene gas-sensing mechanism of (a) pure ZnO NWs and (c) Pt/Pd-ZnO NWs. (b) Energy band diagram of Pt, Pd NPs and ZnO NWs. Reprinted
from Ref. 82 with permission from Elsevier (Copyright 2020).
deposition (ALD). The relationship between the applied voltage (V > 1) thus, a higher gas response. Also, the good selectivity of the sensor to CO
and the increase in the temperature of the sensor due to the self-heating gas was related to a combination of the catalytic effect of Au, the special
effect can be formulated as follows: architecture of the sensor, and the sensing temperature (due to self-
heating). However, the most important factor was the catalytic effect
ΔT = − 1.3575 + 0.120V + 0.1645V2 For V > 1, (9) of Au to CO gas, where a low energy was required for oxidation of CO
where ΔT is the increase in the temperature due to self-heating, and V is over Au NPs [82]. The lowest power for the sensor was found to be 0.81
the applied voltage. Fig. 7(d) shows the variation in responses to CO (50 nW at its corresponding voltage of 1 V whereas the highest power
ppm) for different ZnO shell thicknesses under a 20-V applied voltage. consumption of 8.3 μW was obtained at 20 V. The previous reports that
With increasing ZnO shell thickness from 10 to 30–80 nm, the sensor we reviewed here are all showed energy consumption values from mW
showed increasing responses from 1.22 to 1.34 to 1.62, respectively. to μW. However, the obtained low power consumption in this study
The self-heating effects with different applied voltages from 0 to 20 V clearly indicates that Au/SnO2-ZnO C-S NW sensors are very promising
were checked, and the temperatures obtained 0–20 V were 23–103 ◦ C in the design of portable sensors with extremely low power
(Fig. 7 (e)). The Joule heating process in the SnO2-ZnO C-S NWs can consumption.
contribute to three sources of resistances: (i) in the ZnO grains, (ii) in the In addition to Au NPs, Pt and Pd NPs have been deposited on SnO2-
grain ZnO boundaries, and (iii) through ZnO-ZnO homojunctions (Fig. 7 ZnO core-shell NWs to study their gas-sensing properties under self-
(f)). Accordingly, as the number of NW contacts in the sample increased heating conditions [85,86]. For example, Kim et al. reported
with increasing thickest of the ZnO shell, the corresponding increase in SnO2-ZnO C-S NWs (Fig. 8(a)-(c)) and studied the selective/sensitive
the number of Joule heating sources led to a higher temperature and, detection of toluene gas without using external heating [84]. The SnO2
NWs were synthesized by using a VLS method, whereas the ALD
7
Fig. 7. (a) Schematic presentation of the synthesis procedures for Au-decorated SnO2-ZnO core-shell NWs, (b–c) FE-SEM images of bare SnO2 NWs and Au func
tionalized SnO2-ZnO core-shell NWs, and (d) variation of Au/SnO2-ZnO core-shell NW sensor’s response with the thickness of the ZnO shell. (e) Temperature versus
applied voltage and (f) schematic of the self-heating mechanism in SnO2-ZnO C-S NWs and the corresponding process of resistance generation. Reprinted from Ref. 83
with permission from Elsevier (Copyright 2020).
technique was applied to coat a ZnO shell, followed by γ-ray radiolysis to Thirdly, due to the entangled NW structure of the NWs, it occurs in the
deposit Pt NPs on the sensor surface. The thicknesses of the ZnO shells ZnO-ZnO homojunctions as electrical currents flow through those
was set to 10, 30, and 85 nm for 50, 200 and 500 ALD cycles, respec homojunctions [82]. The sensing mechanism in Fig. 8(e) shows the
tively. Subsequently, the self-heating effect of Pt-decorated SnO2-ZnO formation of heterojunctions between ZnO/Pt and ZnO/SnO2, which
core-shell NW sensors having an 85-nm shell thickness was measured at greatly affect the sensing response.
different voltages from 0 to 20 V. Fig. 8(d) shows thermograph images To further continue their self-heating study, Kim et al. reported on-
obtained at 0, 1, 3, 5, 10 and 20 V. The 10-nm-thick shell shows a chip grown SnO2 NWs Si/SiO2 substrate by using a VLS technique for
negligible self-heating effect whereas the 85-nm-thick ZnO shell sensor ultra-low power consumption sensors in the nW range when operating in
exhibits a quite good self-heating effect. The response of the the self-heating mode [85]. The ZnO shell, which had an 80-nm thick
Pt-decorated SnO2-ZnO core-shell NW sensor with an 85-nm thickness to ness, coated on SnO2 NWs by using the ALD method, after which the Pd
toluene was found to be 3.14. Moreover, the response of the sensor was NPs were coated on the SnO2-ZnO core-shell NWs by using γ-rays radi
explored at applied voltages from 1 to -20 V. The highest response of olysis. The heat produced because of Joule heating is known to be
3.14 was obtained at 20 V, and the lowest response of 1.00 was obtained directly proportional to the voltage and indirectly to the resistance ac
at 1 V. The amount of power consumption of the as-prepared sensor was cording to following formula:
found to be 31 μW at 5 V, which provides promise for applications such
as mobile and portable gas sensors. The mechanism of Joule heating can Q ∝ V2/R (10)
be explained based on mainly three possible sources (Fig. 8(e)). Firstly, Thus, Joule heating can be increased by increasing the applied
the Joule heating occurs inside the ZnO grains as current flows through voltage. The responses of a Pd-SnO2-ZnO core-shell NW sensor toward
them. Secondly, the Joule heating occurs in the ZnO grain boundaries.
8
Fig. 8. (a) Synthesis procedure for realizing Pt-SnO2-ZnO C-S NWs, (b, c) corresponding FE-SEM images, (d) thermographic images of Pt-SnO2-ZnO C-S NW sensors
for different shell thicknesses (10–85 nm) with varying operating voltage (0–20 V), and (e) self-heating and sensing mechanisms. Reproduced from Refs. [84] with
permission from Elsevier (Copyright 2020).
benzene at different concentrations were measured under different the lowest value of 0.99 nW was obtained at 1 V.
applied voltages from 1 to 20 V. With increasing concentration and So far, only n-type MOS materials were discussed for sensing studies.
applied voltages, the response also increased, and the highest response This is due to the fact that in general, p-type MOS-based gas sensors
of 2.62 was obtained for 50-ppm benzene at 20 V. The high selectivity of show lower responses relative to those of their n-type counterparts [95].
the Pd-SnO2-ZnO core-shell NW sensor toward benzene can be attrib However, a few studies of p-type gas sensors operating in the
uted to the interaction between the π electrons of benzene and the d- self-heating mode have been published. Among many p-type MOS ma
band electrons of Pd NPs [76]. A response of 43.13 was obtained for terials, CuO has been investigated for H2S sensing due to its being highly
50-ppm benzene at a temperature of 200 ◦ C. The response of the sensor sensitive to H2S [96,97]. Kim et al. prepared pristine (Fig. 9(a)) and
was mainly attributed to the ZnO shell because the heterojunction bar Pd-functionalized CuO NWs (Fig. 9(b)) for H2S gas sensing in
rier hinders the electron flow from SnO2 to ZnO. Therefore, the majority self-heating mode (1–5 V) as shown in in Fig. 8(c) [86]. The Pd func
of electrons flow through the ZnO shells. The Joule heating in SnO2-ZnO tionalization on the CuO NWs (Pd/CuO NWs) was carried out using
C-S NWs typically occurs in different ways viz. inside the ZnO grains and ultraviolet irradiation (Fig. 9(d)). The Pd-functionalized CuO NW sensor
grain boundaries as well as the ZnO-ZnO homojunctions. The highest was seen to exhibit its best response of 1.894–100 ppm H2S gas at 5 V
value of power consumptions of 22.6 μW was obtained at 20 V whereas which was higher than that of pristine sensor (Fig. 9(e)). The high
9
Fig. 9. (a) Schematic for the preparation of Pd-decorated CuO NWs. TEM micrographs of the as-synthesized (c) CuO NWs and (d) Pd/CuO NWs. (c) Heat generated
under the self-heating condition and the corresponding thermographic image of the CuO NW sensor at 5 V. (d) Self-heating mechanism of the CuO NW sensor
showing the self-heating effects in CuO NWs and CuO-CuO junctions. Reproduced from Ref. [86] with permission from Elsevier (Copyright 2020).
sensitivity of the current sensor was ascribed to the transformation of quicker response/recovery time of ~25 s/~108 s under the same con
CuO to CuS with metallic conductivity during exposure to H2S (Fig. 9 ditions. The higher sensitivity and the faster response of the oxidized
(f)). The change in conductivity from CuO (Eg =1.2 eV) to CuS and the NW array were related to the increased sensing area and the different
catalytic effect of Pd NPs resulted in a high response to H2S gas, in oxidation lengths. The oxidation (PtOx) length of the PtOx/Pt NW array
accordance with literature [97]. The self-heating effects were attributed was 50 nm to ~100 nm, which facilitated a reduction in the response
to two phenomena (Fig. 9(g)), (i) the passing of electrons through the time with the electrode having a nanoscale gap while the higher
CuO NWs and (ii) the CuO-CuO homojunctions network, in which the oxidation lengths (500 nm–1 μm) offered higher surface areas for gas
homojunctions were in direct contact with one another. Thus, the Joule sensing.
heating was generated in the CuO-CuO homojunctions network [83,98], Other than NWs, two dimensional (2D) nanosheets (NSs), especially
leading to temperature increase inside of the sensor and appearance of a 2D layered transition metal dichalcogenides (TMDs) have been also used
sensing signal. for self-heating studies due to their several unique properties [100,101].
In an another experiment, a p-type MOS material was synthesized by In this context, Kim et al. prepared Au NP decorated WS2 NSs (Fig. 10
oxidizing metal NPs such as Pt NPs. Prajapati et al. reported on the use (a)-(b)) for CO sensing in the self-heating mode [87]. Microscopically
gas sensors with a single NW of PtOx and a NW array of PtOx/Pt for H2 analyses which are shown in Fig. 10(c-e), demonstrate the formation of
sensing at RT under a self-heating condition [99]. The diameter of the Pt desired morphology. The actual sensor temperatures were obtained
NW arrays was varied from 10 to 80 nm. For the formation of a single using an IR imaging camera (Fig. 10(f)), and the sensor showed its
PtOx NW, a 60-nm Pt NW was oxidized in an oxygen ambient under a highest response to CO gas at only 2 V (Fig. 10(g)) with a power con
constant voltage. Upon exposure to hydrogen gas, the single NW PtOx sumption of only 28.6 μW. The very low power consumption was related
sensor showed an excellent response (ΔR/Ra × 100) of about 818% to H2 to the intrinsic resistivity of WS2 NSs, which facilitated heat generation
(1000 ppm) at RT under an ultra-low 0.25-V applied voltage. However, within the WS2 NSs. In addition, many WS2-WS2 homojunctions acted as
the NW array of PtOx/Pt showed a higher response (~936%) with a power sources of Joule heating upon application of a voltage. The good
10
Fig. 10. (a, b) Schematic presentation of the synthesis procedures for pristine and Au-decorated WS2 NSs, (c) FE-SEM micrographs of pure WS2 NSs on the sensor
substrate, (d) TEM micrograph of pure WS2 NSs, (e) high-resolution TEM image of Au-decorated WS2 NSs, (f) variation of the temperature (irradiated for 15 s) with
respect to the applied voltage, and (g) response to 50-ppm CO versus applied voltages (irradiated for 1 s). Reproduced from Ref. 87 with permission from Elsevier
(Copyright 2020).
response was related to the catalytic role of Au towards CO gas at low issue of integrating a heater element and to lower the power consump
temperatures. tion. Mostly MOS materials with NWs morphology, including single NW,
Also, MOS materials with nanorod morphology have been used for multiple NWs and networked NWs, have been used for self-heated gas
self-heating studies. For example, Seo et al. and Choo et al. designed self- sensors. However, the design of the individual NW sensors involves
heated gas sensors with high-sensitivity to H2 [102,103]. A complicated process steps and laboratory fabrication methods with low
cost-effective, self-heating (2–8 V), ZnO-based H2 gas sensor was made yield, which are hardly transferable for large-scale production [68].
from ZnO nanorods grown using a hydrothermal process on the surface Also, core-shell NWs are very promising for use in the self-heating mode
of indium tin oxide (ITO) [103]. Joule heating was mostly generated due to maximization of the interfaces between the core and the shell.
inside the ITO whereas ZnO acted as a resistor to modulate the electrical Sensing materials decorated with noble metals can operate with low
resistance of the sensor. At 4 V, evidence of Joule heating in the sensor power consumptions due to their high sensitivity resulting from the
was obvious, and with further increases in the operating voltage, higher presence of the noble metals. Table 1 shows the properties and the
temperatures were obtained for the sensor. At a maximum 8 V, the power consumptions of some self-heated gas sensors reported in the
working temperature was 75 ◦ C, and the highest gas response to H2 was literature.
the result. However, no selectivity study was performed.
The above section can be summarized as follows: the reasons for
operating the gas sensors in the self-heating mode are to overcome the
11
Table 1
Summary of different self-heating gas sensors showing their sensing properties and power consumptions.
Sensing materials Target gas and conc. (ppm) Power consumption Applied voltage (V) Sensitivity (S) [Ra/Rg or Rg/Ra Ref.
*[(Ra-Rg/Ra) × 100]
Ag decorated SnO2 NWs H2S (0.5) 2 mW – 21.2 [33]

SnO2 NW networks NO2 (1) 1 μW – 3.2 [38]
SnO2 NW NO2 (10) 10 μW – 1.3 [38]
Pt-coated W18O49 nanowire networks H2 (50) 30–60 mW 6 ~1.1 [61]
SnO2 NWs C2H5OH (100) 10 mW – 3.75 [63]
SnO2 thin films CO (1000) 0.1 W 10 (ac) 1.01 [64]
SnO2 individual nanowires (r < 45 nm) NO2 (0.5) 27 μW – 1.01 [66]
SnO2 individual NW NO2 (40 ppm) 35 μW 25 V 21.3 [67]
SnO2 multiple NW NO2 (40) 90 μW 40 V – [67]
SnO2 networked NW NO2 (40) 56 μW 40 V – [67]
Pd-SWCNTs CH4 (6) few μW – 1.02 [68]
networked SnO2 NWs NO2 (2.5) 25 mW 1 25.6 [74]
Pt-coated SnO2–ZnO core–shell NFs C7H8 (50) 31 _W 3 1.41 [84]
Pd functionalized SnO2-ZnO core-shell NWs C6H6 (50) 22.6 μW 20 1.62 [85]
Pd functionalized CuO NWs H2S (100) - 5 1.894 [86]
Au-decorated WS2 nanosheets CO (50) 28.6 μW 40 1.48 [87]
Pd functionalized carbon NWs H2 (1000) 30 μW – 1.2 [102]
WO3 nanocolumnar thin films NO2 (1) 21.6 μW 5 ~130 [104]
Ti NPs decorated MWCNTs O2 10–100 μW 0.5 1.1 (10 mTorr) [105]
Pd functionalized Si NWs H2 (10,000) Few μW 1.7 1.65* [106]
Pd functionalized carbon NWs H2 (1000) 30 μW – 1.2 [107]
Suspended SWCNTs NO2 (1) 2.9 μW 5 1.8 [108]
different sensor arrays on a single sensor platform that can be utilized for
mass-production at a low cost [113]. Nanoscale MOS materials inte
grated with MEMS technology are widely employed in gas sensing ap
plications due to the drastically reduced size, low cost and significantly
lower power consumption of such devices [114–116]. In comparison
with traditional MOS-based gas sensors (Fig. 12(a)), MEMS-based gas
sensors that use MOS materials typically consist of three basic compo
nents: (i) a micro-heater, (ii) a sensing material in the form of a thin film
(receptor layer), and (iii) interdigited electrodes (Fig. 12(b)). The
micro-heater embedded in the substrate layer (suspension), a dielectric
layer or an insulation layer, a passivation layer, and a microheater
element, as shown in Fig. 12(c-e), are components of a conventional
MOS gas sensor [117,118]. Different materials, such as platinum (Pt),
nichrome (Ni) and tungsten (W), can be used for the fabrication of the
heater part [119–121]. Five categories of microheater geometries are
typically used: rectangular, square, circular, irregular shapes (like
Fig. 11. Recent progress on the miniaturization of sensors with respect to their
honeycombs, drive wheels or others), and 3D structures. The most
power efficiency. Reproduced from Ref. 112 (MDPI) under the license of cre
ative commons attribute (https://creativecommons.org/licenses/by/4.0/).
widely reported structure is the meander shape with either a square or a
rectangular pattern [122]. Microheaters can be categorized into
different configurations, such as a closed membrane, a suspended
3. Low-power MEMS-based gas sensors
membrane or a bridge (Fig. 12(c)–(e)). In all of them, the substrate just
below the sensing region is etched away. Among them, the suspended
During the fabrication of sensing devices, MOS sensors are connected
membrane substrate (Fig. 12(d)) is the most popular because of its much
to a heater, which is necessary to activate the sensing reaction between
reduced power consumption [123]. The suspended membrane may
the target gas and the sensing material. Therefore, many MOS-based
either be released from the front side (Fig. 12(f)) or the back side (Fig. 12
commercial gas sensors use heater resistors to warm the sensing sur
(g)). The main aim in making bridge/diaphragm architecture is to
face to the desired temperature [109]. However, the power consumption
reduce the heat loss through air, which has a low thermal conductivity:
of such gas sens0rs is high [110], which limits their application to
0.026 WK− 1 m− 1 at 20 ◦ C, by using thermal isolation, thereby inducing
smartphones and portable electronic devices. Therefore, a micro heater
low power consumption. The back-side etching of a substrate is good
with low power consumption can play a vital role in overcoming the
due its simplicity compared to front side etching because the front side
above issue [111]. The recent advances in different fabrication tech
etching for creating the cavity needs extra protection of the structure
nologies have lead to the downsizing of sensing chips and heater re
layer or the sacrificial layer.
sistors, resulting in tiny, reduced-power gas sensors (Fig. 11). Especially,
MOS-based MEMS gas sensors were first realized in the early 1990s
the micro-electromechanical system (MEMS) has enabled very compact,
and were derived from the so-called micro-hotplate devices [124]. Many
low power consuming (a few tens of mW), MOS gas sensors to be
reports on MOS-based MEMS gas sensors have been published [111,
fabricated [112].
125–127]. For example, Hsueh et al. fabricated a transparent
Gas sensors based on MOS materials can be integrated into MEMS
MEMS-type gas sensor (Fig. 13) based on ZnO NWs (length: 2.5 μm,
platforms to achieve miniaturized and portable sensing devices with
diameter: ~75 nm) synthesized using a hydrothermal method as the
very low power consumptions. MEMSs are electro-mechanical systems
sensing material, ITO as a transparent electrode, and a micro heater
with a 3D geometry. They are constructed on silicon-wafer platforms by
[127]. The highest power consumption at an applied voltage of 6.73 V
using microelectronic fabrication of a photolithography method and
was only 124 mW whereas the maximum power consumption obtained
post-process techniques. These processes allow designers to accumulate
at an applied voltage of 11.55 V was 386 mW. The temperature obtained
12
Fig. 12. (a) Schematic diagrams of all the components of a conventional MOS gas sensor, (b) a MEMS-based MOS gas sensor. Schematic diagrams of different
configurations of a MEMS based MOS gas sensor, (c) closed, (d) suspended, and (e) bridge membrane (e), and schematic diagrams of suspended microheater with (f)
front side, and (g) back side etching. Reproduced from Ref. 118 with permission from MDPI (Copyright 2020).
sensor consumed only 100 mW of power. At 300 ◦ C, the sensor exhibited

a high sensing response [(ΔR/Ra) × 100] of ~275% to 50 ppm of
acetone. The enhanced gas-sensing performance was attributed to the
charge carrier modulation at the surfaces of ZnO and CuO, the barrier
height modulation at the ZnO-CuO interface, the presence of defects in
the interfaces between ZnO and CuO, the catalytic effects of CuO, and
the higher dipole moment of acetone relative to those of other gases.
MOS-decorated gas sensors also have been used in MEMS configu
rations. For instance, Yuan et al. reported a MEMS-based acetone sensor
made from CeO2 nanodots decorated on WO3 NWs, prepared through a
hydrothermal and subsequent thermal decomposition [129]. The sensor
exhibited a response (Ra/Rg) of 1.30–500 ppb acetone with good sta
Fig. 13. Schematic illustration of a ZnO NW-based MEMS sensing device. bility, which indicates that this sensor can be used to diagnose diabetes
Reproduced from Ref. 127 with permission from Elsevier (Copyright 2020).
via breath analyses. The sensing mechanism was related to the high
surface area of the gas sensor, the fast carrier transport of the WO3 NWs,
at 6.73 V was 150 ◦ C, and that obtained at 11.55 V was 350 ◦ C. The the formation of WO3-CeO2 heterojunctions, and the existence of large
sensing results showed that the response to NO gas was higher than the numbers of oxygen vacancies in CeO2.
responses to other gases due to the fact that the bond energy of NO (N–O In summary, even though gas sensors based on MEMS technology can
= 200 kJ/mol) is lower than those of other gases. Also, a operate with reduced power consumption, the slurry-based drop coating
blue-light-emitting diode (LED) was integrated into the MEMS sensor, of sensing materials on the small sensing areas of MEMS micro hot plates
and its lighting effects on the gas-sensing characteristics at RT were is an extremely difficult task. Furthermore, fabrication of MEMS-based
investigated. When the LED was switched on, the sensor current sensing devices on a large-scale has difficulties such as low yield and
increased while it decreased when the LED was switched off, which was large sample-to-sample deviation, which ultimately limit their practical
related to the presence of defects in the ZnO NWs. A large number of use. One good strategy to deal with this is to deposit the sensing material
electrons were generated by LED-emitted light, and the presence of by using advanced physical techniques such as sputtering, which is a
defects and photo-generated electrons led to an enhanced response to simple technique, to integrate the sensing materials on micro-hot-plate
NO gas. platform [130].
MOS composites have also been used in MEMS configurations to
enhance the sensitivity of MEMS-based gas sensors. Behera et al. syn
4. Low or room-temperature operated MOS gas sensors
thesized p-n ZnO-CuO nanoflake heterojunction nanostructures based
on a MEMS platform (Fig. 14 (a) and (b)) [128]. The simulated tem
So far we reviewed the MOS-based gas sensors in self-heating mode
perature distribution profile of the microheater indicated that the heat
without external heater. Mostly, various MOS materials with NW
was uniform throughout the substrate and confined within the sensor
morphology have been reported for operation in self-heating mode.
platform (Fig. 14(c)). At an increased sensing temperature of 259 ◦ C, the
However, a very few reports on other kinds of morphologies based on
13
Fig. 14. (a) Schematic and (b) photographic image of a MEMS-based gas sensor. (c) temperature distribution of the microheater. Reproduced from Ref. 128 with
permission from Elsevier (Copyright 2020).
self-heating method for gas sensing application have been also published the surface of the sensor and electronic interactions occur between
[87,102,104]. target gases with the oxygen ions of the sensor [153–155].
Conventional MOS-based gas sensors usually operate at high tem In addition to n-type MOSs, p-type MOSs has also been studied for RT
peratures ranging from 100 to 450 ◦ C in order to achieve enhanced gas sensing. For instance, Li et al. reported a highly sensitive and se
sensing performance because of their larger band gap [77,131], which lective H2S gas sensor using porous CuO nanosheets, synthesized using a
leads to serious problems such as high-power consumption and increase hydrothermal method [135]. The sensor exhibited a response of 1.25
of overall price of the gas sensor due to need for the heater. Thus, RT towards 10 ppb H2S with response/recovery time of 234 s and 76 s and
operation of gas sensors is highly desirable to minimize the risk of gas excellent selectivity to H2S. According to the literature p-type CuO is the
explosion, reduction of energy consumption, increases sensor life and dominant material for H2S sensing [156]. The sensing mechanism was
possibility of integration into smart phone devices [132,133]. Recently, mainly related to the transformation of semiconducting CuO to metallic
many strategies have been carried out to enhance the sensing properties CuS. In fact, H2S molecules can react with CuO to form CuS, based on the
at MOS gas sensors RT such as morphology engineering of pristine MOSs following reaction [156].
[134–136], noble metal NPs-decorated MOSs [137,138], doped MOSs
[139,140], construction of heterojunction structures [141,142], hybrid H2S (g) + CuO (g) → CuS (s) + H2O (g) (11)
composites with conducting polymers [143], carbon materials The transformation to CuS was confirmed by using XPS analysis,
[144–146] and 2D materials such transition metal chalcogenides, metal where after exposure to H2S gas a new peak related to the Cu 2p3/2 state
carbides [147,148]. Also UV-irradiation is a good technique to reduce at 930.8 eV appears which can be attributed to CuS. Similar transition to
the sensing temperature [149,150]. In following section we discuss metal sulfide also has been reported for In2O3 gas sensor [157].
about low temperature or RT gas sensors based on MOS materials.
4.2. MOS modified with noble metal NPs
4.1. Pristine MOS gas sensors
Noble metal NPs (Au, Ag, Pd, and Pt) not only can remarkably
It is known that morphology greatly affects the gas sensing proper enhance the sensitivity, shorten the response/recovery times and
ties, and therefore various morphologies have been used for sensing enhance the selectivity, but also can decrease the operation temperature
studies [151]. For example, Wang et al. prepared WO3 hierarchical of gas sensor. Because at RT, the detection of a few gases like CO and H2
hollow spheres by a facile hydrothermal method and explored its NO2 by pristine MOS sensor is difficult. But, this issue can be solved by
sensing properties at RT [152]. The sensor exhibited a high response modifying the surface of the sensor using these noble metal NPs. Hence,
(Rg/Ra) of 15.1 to 300 ppb NO2 gas with excellent selectivity and the noble metal functionalization is regarded as one of the best ap
moderate response/recovery times (670 s/2940 s) and good repeat proaches for enhancing gas sensing properties [78,158]. For example,
ability. The high NO2 sensing performance of the sensor was related to Arunkumar et al. [159] prepared ZnO nanostars using a hydrothermal
the large surface area, presence of high oxygen vacancies and electronic followed by the decoration of different wt% of Au NPS (as shown in
interactions which occurred between NO2 gases with the oxygen ions on Fig. 15(a–b).) The ZnO nanostars with 3 wt% Au NPs showed highest
14
Fig. 15. (a–b) TEM images of 3 wt% Au loaded ZnO nanostars, and representative energy band diagram of pristine and Au loaded ZnO nanostars before (c–d) and
after CO exposure (e–f). Reproduced from the ref 159, with the permission from Elsevier, copyright 2020.
surface area among other morphologies such as ZnO nanoflowers, respectively. The enhanced ethanol gas sensing was attributed to the
marigold and nanorods. The Au-ZnO nanostars also exhibited excellent formation of depletion layer at the p-n junction and catalytic activity of
sensitivity (Rs = 35) towards 500 ppm CO with a very fast response/r the NiO [140].
ecovery times (41 s/40 s) at RT and excellent selectivity to CO among Another p-n heterojunction sensor was prepared by an electro
other interfering gases. Due to the spillover effect [160] of Au NPs, the spinning method using mesoporous In2O3-CuO composite nanofibers
thickness of EDL formed at the interface between Au and ZnO increases (Fig. 16(b)–(c)), with a high surface area of 48.7 m2/g. Due to a meso
(Fig. 15(c–f)) and upon exposure to CO gas, significant reduction in the porous morphology and high surface area, as well as formation of p-n
thickness of EDL, contributing to the sensing signal. Moreover, the hi heterojunction (Fig. 16(d)), the sensor showed a response 1.5–100 ppm
erarchical structure with numerous channels provided plenty of NH3 at RT with good selectivity and fast dynamics [141].
adsorption sites for CO gas molecules [161].
4.4. MOS structure modified with 2D materials

4.3. p-n heterojunction nanostructures
Recently, various 2D nanomaterials, such as graphene and its de
Composite structures comprising of n-p heterojunctions are highly rivatives, transition-metal dichalcogenides (TMDs), black phosphorous
demanded in gas sensing application due to their synergistic effects [84, and transition-metal carbides/nitrides (MXene), have been used for the
94]. The sensing performance can be greatly improved due to the elec fabrication of RT gas sensors [145]. However, their RT sensing proper
tronic sensitization at p-n heterojunctions and broadening of EDL on the ties need to be enhanced in terms of sensitivity, selectivity and respon
interfaces between the sensing materials (Fig. 16(a)). se/recovery [93,146,163,164]. The combination of these 2D materials
An ethanol sensor based on p-n NiO/SnO2 nanocomposite reported with a MOS structure has led to significant improvements in the sensing
recently [139]. The sensor exhibited a high sensitivity of (Ra/Rg=140) to properties [87].
100 ppm ethanol at RT with fast response/recovery times of 23 and 13 s, Due to its excellent conductivity, high surface area, and unique 2D
15
Fig. 16. (a) Schematic representation of the energy-band diagrams at heterojunction interfaces of different types of MOS heterojunctions. Reproduced from Ref [27]
with the permission from Elsevier, Copyrights 2020. (b–c) TEM images of CuO-In2O3 composite nanofibers, and (d) Schematic of the sensing mechanism. Reproduced
from Ref [141] with the permission from Elsevier, 2020.
structure, reduced graphene (rGO) has been recognized as a promising materials were aligned in the sensor electrodes to form uniform multi
sensing material [165,166]. Especially, it is used in composite form to channel sensing devices. The sensor exhibited an ultrahigh response of
enhance its sensing properties. For example, a nanocomposite with a 34.41 toward 5 ppm of NO2 at RT. The high sensing performance was
rGO-ZnO-SnO2 heterostructure was synthesized by using the hydro related to the large sensing area resulting from the presence of rGO, to
thermal method [167]. The as-prepared ternary composite sensor the 3D nature of the sensing layer, and to the high electron transport
exhibited a response (ΔR/Ra × 100) of 141% towards 5 ppm of NO2 at between rGO and Fe3O4-SiO2.
RT. The presence of rGO led to rapid electron transfer between ZnO and Transition-metal dichalcogenides (TMDs) such as molybdenum di
SnO2. Furthermore, the formation of p-n and n-n heterojunctions sulfide (MoS2) have grabbed tremendous attention due to their having
contributed to the enhanced NO2 sensing characteristics. high stability, numerous surface active sites for functionalization and
In another study, Ma et al. reported RT gas-sensing three-dimen gas adsorption, and good conductivity at RT [147,169]. However, the
sional (3D) Fe3O4-SiO2-rGO core-shell spheres synthesized using elec pristine MoS2 gas sensors exhibit low sensitivity and slow dynamics at
trostatic self-assembly, followed by thermal reduction [168]. The RT [170]. Accordingly, it is mostly used in a composite form. For
as-prepared 3D Fe3O4-SiO2-rGO nanosphere suspensions (0.5 mg/mL) example, Han et al. reported the fabrication of MoS2/ZnO hetero
were dropped onto the sensor chip under a magnetic field (0.28 T) structures via a wet chemical route [171]. The sensor showed a response
applied perpendicular to the electrodes, and after evaporation, the (ΔI/Ia) of 30.50 towards 5 ppm of NO2 with an ultrafast response time
16
Fig. 17. (a)–(d) Wearable gas sensor based on RGOCY. Reproduced from Ref. 208 under the license of creative commons attribute (https://creativecommons.org/
licenses/).
(40 s). The sensing mechanism was explained on the basis of the syn [184–186], many MOS/conducting polymer (CP) composites have been
ergistic effects of the unique 2D/0D morphology and the formation of used for such purposes. CPs such as polyaniline (PANI), polythiophene
p-n junctions between ZnO and MoS2 [172]. In another study related to (PTh) and polypyrrole (PPy) are the most common polymers for RT
MoS2, Chen et al. reported the surface functionalization of MoS2 by Au gas-sensing studies due to their unique electrical and optical charac
NPs for selective detection of acetone at RT [173]. The sensor exhibited teristics, low cost, ease of fabrication, and flexibility [187–189]. Most
high a response to acetone gas, which was related to the strong CPs have good sensitivity to ammonia gas, but in pristine form, their
adsorption of acetone molecules on the Au-MoS2 sensor and to the high recovery times are long; thus, they are mostly used in composite form
catalytic activity of Au NPs towards acetone. with MOS structures. For example, Beniwal et al. demonstrated NH3
Another category of 2D materials with sheet-like or layered SnO2/PPy electrospun composite sensors [190]. The sensor showed an
morphology is known as MXenes, which have a general formula of excellent response (ΔR/Ra) of 57% with a short response/recovery time
Mn+1AXn, (MAX phase), where M stands for a transition metal, A is a of 18 s/30 s for 100 ppb of NH3 at RT. The intrinsically good sensitivity
IIIA or IVA element, and X is N and/or C with n = 1, 2, or 3 [174–177]. of SnO2 to NH3, along with formation of p-n heterojunctions, led to the
The advantages of these materials are high conductivity, high surface enhanced response to NH3 at RT. Furthermore, PPy has a -NH- group,
area due to the unique 2D morphology, and excellent flexibility, which which can easily interact with NH3 gas, thereby increasing the electrical
make them attractive materials for many applications, including gas resistance and, hence, the gas response. PPy/MnO2 and PANI/Fe2O3 are
sensing [176–179]. Some studies related to the gas-sensing properties of other examples of composites used for RT gas-sensing studies [191,192].
a pristine Mxene and its composites with a MOS structure have been Recently, a novel CuO-Chitosan nanocomposite H2S gas sensor was
published [179–183]. For example, Tai et al. designed an ammonia gas introduced by Fajr et al. [189]. The sensor revealed a fast response of 14
sensor made from Ti3C2Tx and TiO2 composite nanostructures [148]. s and a high response (ΔR/Ra) of 217.89% for 100 ppm of H2S gas at
TiO2 NPs were deposited on the synthesized Ti3C2Tx nanosheets to 40 ◦ C. They also measured the power consumption of the sensor and
fabricate TiO2/Ti3C2Tx nanosheet composites. The fabricated gas sensor found that it showed a power consumption of 0.45 W at 40 ◦ C. The
exhibited a higher response to ammonia relative to other gases at RT. formation of heterojunctions and the catalytic effect of CuO contributed
The enhanced NH3 sensing response of the sensor was explained using to the sensing signal.
the model of self-built electric-field (space-charge layer) regulation.
Upon intimate contact between Ti3C2Tx and TiO2, electrons in the
conduction band of TiO2 migrated to Ti3C2Tx due to its excellent 4.6. MOS treated with UV-irradiation
metallic properties and to the higher work function of Ti3C2Tx, leading
to a self-built electric field (Schottky barrier) at their interface. In air, the A good strategy for decreasing the operation temperature of gas
density of holes on the surface of Ti3C2Tx increases whereas the number sensors is UV illumination. When the energy of UV light is equal or
of electrons on the surface of TiO2 decreases because the electrons are higher than the band gap energy of the sensing material, photogenerated
consumed by the generated ionized adsorbed oxygen, resulting in a electrons and holes can be produced by the absorption of UV light. In
weakening of the self-built electric field due to the increased number of fact, the energy required to excite these electrons and holes is supplied
holes in Ti3C2Tx and decreased resistance of TiO2/Ti3C2Tx. On the by the light, instead of by heat. Furthermore, illumination facilitates the
contrary, in NH3, the self-built electric field was strengthened due to a chemisorption of oxygen molecules on the surface to generate more O-2
decrease in the number of holes on the surface of Ti3C2Tx and an in by improving the chemical activity of the surface [116] at RT as follows
crease in the number of electrons on the surface of TiO2 (4NH3 + 5O–2 → [150,160–162]:
4NO + 6H2O + 5e–), leading to increased resistance. hν → h+ + e- (12)
O2 + e− (hν) → O-2(hν) → O–2 (hν), (13)

4.5. MOS structure modified with conducting polymers
where ν is the frequency of the illuminated light and h is Planck’s
In addition to the MOS/rGO nanocomposites used for sensing studies constant.
17
Fig. 18. (a) Schematic illustration for the fabrication of an In2O3-rGO film on a flexible PI substrate by using laser writing. (b, c) Photographs of the flexible PI.
Reproduced from Ref 185 with permission from Elsevier, 2020.
Many reports about RT operation of gas sensors under UV illumi cannot be used in applications that require high flexibility. For example,
nation [117,193–195] have been published. For example, Cui et al. re in some applications such as personal use, a gas sensor must be flexible
ported ZnO nanostructures with different morphologies (nanofibers, under mechanical deformations and must have properties making it
nanoflowers, nanoplates) for HCHO detection under illumination with suitable for wearing. Flexible gas sensors are realized on flexible sub
UV light at RT [196]. The ZnO morphology played a significant role in strates, and upon stretching, titling or bending, their properties should
the sensing capacity, and the ZnO nanofiber sensor was found to display not change significantly [197]. Flexible gas sensors with low weight, low
a high response of 12.61 (Ig/Ia) to 100 ppm of HCHO under illumination price, high flexibility, high stretchability, and high conformability can
with 365-nm UV light at RT. Initially, under exposure to UV light, act as good platforms for wearable gas sensors and has significance in
chemisorbed oxygen ions are formed due to the removal of electrons monitoring in ambient atmosphere at RT [198–200]. Wearable sensors
from the conduction band of ZnO, resulting in the formation of a with integrated wireless technology can be integrated to an end-user
depletion layer. The photo-induced oxygen O−2 ions (hν) are weakly with the Internet of Things (IoT) and offer real-time information for
bound to ZnO and can be removed just by turning-off the UV light. When personal use [201], which has opened a new path for smart wearable
a ZnO sensor is exposed to HCHO, the following reaction occurs: devices. Different flexible substrates, such as polyethylene-terephthalate
(PET) [202], polyimide (PI) [203,204], Kapton® [205], have been used
O−2 (hν) + HCHO (g) → CO2 + H2O + e− . (14) for the realization of flexible and wearable sensors. Graphene and its
The release of electrons and the desorption of oxygen species lead to derivatives have been shown to be ideal candidates for flexible gas
a reduction in the thickness of the depletion layer and a decrease in the sensors due to their high mechanical strength, good stability, high car
electrical resistance [196]. The sensing enhancement in ZnO nanofibers rier mobility, and good flexibility [206,207]. Moreover, gas sensors
was related to the surface area (9.61 m2/g) of this sensor with a fibrous based on fibers or textiles have been investigated due to their potential
structure being larger relative to those of other morphologies. applications in wearable devices. For example, Yun et al. reported a
In this section, we discussed various strategies to enhance the RT bendable and washable electronic-textile (e-textile) gas sensor based on
sensing properties of MOS-based gas sensors. In general, different stra a composite of RGO-decorated cotton yarn, the so-called RGOCY (Fig. 17
tegies such as composite made using n-n MOSs or p-n MOSs, decoration (a)) [208]. The sensor was able to sense NO2 gas at RT. Fig. 17(b)–(e)
with noble-metal NPs, and morphology engineering, as well as hybrid show the performance of the fabricated gas sensor under different
composites with carbon materials or CPs, have been used to realize RT conditions, such as bending (bend radius of 1.0 mm) and straightening;
gas sensors. Gas sensor operating at low temperatures with little or no even after washing with a detergent, the sensor showed stable sensing
power consumption can be used for different applications. In the next properties, demonstrating its excellent performance under different
section, we will discuss the most important applications of gas sensors , conditions. Moreover, after 1000 bending-straightening cycles, the
namely, flexible and wearable gas sensors. sensor exhibited stable electrical and sensing properties. The stability
under washing was attributed to the chemical against water and deter
5. Applications of low or RT gas sensors gent and to the mechanical resistance to shearing resulting from friction
between the yarn and the magnetic stirrer during the washing of the gas
5.1. Flexible and wearable sensors sensor.
Lee et al. first introduced a flexible hybrid sensor based on graphene
Considering the types of substrates used for gas sensor fabrication, fibers and Ti3C2Tx Mxene fabricated by using a wet spinning process
gas sensors can be divided into flexible and non-flexible (rigid) gas [150]. Initially, Ti3C2Tx MXene was synthesized, after which it was
sensors. The non-flexible sensors, which are currently the most common dispersed with a GO suspension to be drop casted onto the Si/SiO2
types, are fabricated on rigid substrates. However, they are rigid and substrate to realize a composite sensor. After thermal activation at
18
Fig. 19. (a) Schematic of a flexible SWNT-Fe2O3 sensor bent from 0◦ to 180◦ . (b) Response of a SWNT-Fe2O3 composite sensor to 20-ppm H2S at different bending
angles from 0◦ to 90◦ –180◦ to 0◦ . Reproduced from Ref. 212 with permission from Elsevier (Copyright 2020).
Table 2
Gas-sensing properties of RT-based gas sensors.
Sensing materials Target gas/concentration Response time/recovery time Response [Ra/Rg or Rg/Ra] or *[(Ra-Rg/Ra) × 100] Ref.
WO3 hollow spheres NO2 (0.3 ppm) 670 s/2940 s 15.1 [152]
CuO nanosheets H2 S (0.01 ppm) 234 s/76 s 1.25 [ 135]
Au loaded ZnO nanostars CO (500 ppm) 41 s-/40 s 55.3 [160]
Pt-PdO NWs H2 (10 ppm) 166 s 62%* [163]
NiO-SnO2 nanocomposites C2H5OH (100 ppm) 23 s/13 s 140 [139]
In2O3-CuO composite nanofibers NH3 (100 ppm) 2 s/- 1.57 [141]
ZnO/SnO2-rGO nanocomposite NO2 (5 ppm) 32 s/92 s 141%* [167]
Fe3O4@SiO@rGO nanospheres NO2 250s/– 429% [168]
1 ppm
MoS2/ZnO p-n heterojunction NO2 (5 ppm) 40 s/– 30.5% [172]
Au-loaded MOS2 Acetone (120 ppm) 105 s/160 s 42.2% [173]
TiO2/Ti3C2Tx NH3 (10 ppm) 33 s/277 s 3.1% [148]
Mxene composite
SnO2/PPy nanofibers NH3 (0.1 ppm) 18 s/30 s 57% [190]
UV irradiated ZnO nanofibers HCHO (365 nm UV light) – 12.61 [73]
rGO/Ti3C2Tx NH3 (100 ppm) 4.2 min/13.3 min 6.7% [150]
Flexible composite
In2O3/rGO composite NO2 (1 ppm) – 31.6% [185]
PEDOT:PSS/rGO nanocomposite (NH3) – 18.9% [209]
1000 ppm
SWNT/Fe2O3 composite films (NH3) 250 s/350 s 4% [212]
200 ppm
200 ◦ C, the composite Ti3C2Tx/GO was reduced to Ti3C2Tx/rGO, and its of NO2 gas at RT, which limit its applications in real situations.
gas-sensing properties at RT were measured. The sensor displayed an In addition to the composites made from rGO/MOS [185], rGO/M
enhanced response to NH3 (ΔR/R0 × 100 = 6.77%) with excellent xene [183] and rGO-cotton Yarn [208], CP-based composites [188,209]
flexibility and stability, enabling its use in portable and wearable have also been studied for flexible, wearable sensors at RT. PEDOT:PSS
sensing devices. At RT, the band gap of the Ti3C2Tx/rGO composite was is a conjugated polymer that is widely used for flexible and printed
widened from 1.05 eV to 1.57 eV, which had a positive effect on its electronics due to its good electrical conductivity, high transparency,
sensing properties. Also, the optimum content of Ti3C2Tx in the and good processability. Seekaew et al. demonstrated a flexible gas
Ti3C2Tx/rGO composite was 40 wt%. For higher amounts of Ti3C2Tx, the sensor based on a PEDOT-PSS/graphene nanocomposite [209]. Yama
band gap decreased, leading to a weak gas response due to the simul zoe et al. demonstrated a flexible gas sensor based on a
taneous increase in the density of charge carriers. PEDOT-PSS/graphene nanocomposite [78]. The sensing film was
Many reports on rGO composite gas sensors with good flexibility deposited on a flexible substrate by using ink-jet printing. The ink for
have been published [183,184]. You et al. reported a flexible sensing ink-jet printing was prepared using a PEDOT:PSS and graphene solution.
device made of a composite film of graphene and In2O3 for NO2 sensing The sensor showed high selectivity to NH3 at RT and exhibited a p-type
at RT [185]. They designed a direct laser writing (DLW) process to conducting behavior. The increased NH3 sensing response for increased
integrate the In2O3-RGO sensor. The coated In2O3-GO film on a flexible bending was related to the swelling effect of the sensor, where NH3 gas
substrate was converted to In2O3-RGO by using a CO2 laser and a pro molecules diffused into the graphene-PEDOT-PSS layer [210]. The
grammable scanning procedure (Fig. 18 (a)-(c)). One of the benefits of enhanced sensing properties of the sensor were related to the direct
laser treatment is that it makes the sensor conducting due to the photo charge-transfer process between the graphene-PEDOT-PSS surface and
reduction of GO. Even though the initial In2O3-GO film was an insulator the NH3 molecules due to the improved interactions via π electrons, the
with high resistance, after laser treatment it was conductive. Although high specific surface area due to the presence of graphene with a
the In2O3-RGO composite sensor showed a good sensitivity to NO2 gas, sheet-like morphology, and the swelling due to the diffusion of NH3
its response and recovery times were ~ 4.2 min/~ 13.3 min to 500 ppb molecules into the graphene/polymer chain matrix [211].
19
Scheme 1. An overview of resistive-based gas sensors based on their energy consumption point of view.
Other than the rGO, another carbon material, namely, a single wall materials with NW morphology have been reported for operation in self-
carbon nanotube (SWCNT), has been utilized to realize flexible gas heating mode. Thus, there is much room available for the future
sensors due to its having a high surface area, porous structure, high development of other morphology based self-heated gas sensors.
conductivity, and strong affinity for the adsorbed gas molecules. For Although, the self-heated gas sensors could able to show the power
example, Hua et al. prepared SWNT-Fe2O3 composite films by combi consumption in the range of nW level, however, the response value of
nation of CVD and subsequent heat treatment in air [212]. As presented most the sensors in this category are very less, which needed to be
in Fig. 19(a), the gas sensor was deposited on a flexible plastic substrate, studied further.
and it was able to be bent to large angles (90◦ and 180◦ ) and then Utilization of UV light is another technique used to decrease the
recover to its initial flat shape. The gas sensor’s responses to 20 ppm of operating temperature of gas sensors. UV light with energies higher than
H2S under different bending angles at RT are presented in Fig. 19(b). The the band-gap energy of the sensing layer can excite electrons to the
sensor was deformed from a straight to a bent shape 16 times. Under all conduction band, and reactions of the electrons with oxygen and target
conditions, the sensor showed almost similar responses to H2S gas. gases can enhance the response of the sensor at RT. However, posi
RT gas sensors are in high demand for different applications because tioning a source of UV light just above the sensing layer is not always
no external energy is required for their operation. Table 2 summarizes possible due to size limitations and economic considerations. Sensors
the RT gas-sensing properties of resistive-based gas sensors. The table that can work at RT without the need for UV light or operate in the self-
clearly demonstrates that different sensing materials, whether in pris heating mode do not need any external heater and, therefore, hold
tine, composite or decorated form, with various morphologies have been promise for energy-saving purposes. In addition to materials,
successfully used for RT gas sensors. morphology greatly affects the sensing properties of sensors that work at
RT. Among different strategies to improve the gas-sensing properties of
6. Conclusions, challenges and future perspectives RT based gas sensors, the noble-metal functionalization and construc
tion of heterojunction nanostructures are widely used. However, the
In this comprehensive review paper, we discussed the recent prog operation of a sensor at RT has some challenges. The catalytic and
ress in the field of energy-saving gas sensors in terms of various sensing sensitization effects are the main reasons for enhancement of sensitivity
materials, sensing mechanisms, and strategies used to save energy. Due and selectivity of RT gas sensors. On the other hand, the synergistic
to the fast development of 5G technology and IoT and to further im effects of heterojunctions are the primary reason of the high sensing
provements of life service, in the near future, energy-saving gas sensors properties of p-n heterojunction based RT gas sensors. However, the
will be in high demand and will be extensively integrated into common humidity presence in the RT sensing ambient can significantly reduce
electronic devices, such as smartphones, tablets, smart watches and so the sensitivity of a gas sensor. Furthermore, most often the reactions
on. For these applications, realization of flexible, highly sensitive, se cannot be completed at RT; accordingly, the response at RT is lower
lective, stable and cheap gas sensors with fast response and recovery relative to those at higher temperatures.
times are in great demand. MOS-based MEMS gas sensors are another choice as they have simple
Self-heating is a promising strategy for MOS-based gas sensors, architectures, are easy to fabricate, and are efficient in term of energy
especially for MOS materials with NW morphology. Operation of gas use. In fact, the use of MEMS gas sensors not only can significantly
sensors in the self-heating mode can greatly decrease the power con decrease the final dimensions of the gas sensors but can also lead to
sumption from several μW to nW level. Such reductions in the power reductions in power consumption in gas sensors and electronic devices.
consumed can remarkably increase the sensor life and save a great However, considering the power consumption of the above studied gas
amount of energy. Single, ordered, and networked NWs can be used for sensors, MEMS based gas sensor still behind the self-heated gas sensors
this purpose. However, synthesis of networked NWs is easier than that of (Scheme 1). One of the problems of MEMS gas sensors is they still use the
single or ordered NWs, and as a result, currently, it is the most widely external heater and gas sensing measurement still requires the elevated
used morphology for self-heating gas sensors. However, mostly MOS temperatures for the operation. Hence, it is still challenging to overcome
20
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24
Hyoun Woo Kim joined the Division of Materials Science and

Engineering at Hanyang University as a full professor in 2011,
after 10 years working at Inha University. He received his B.S.
Sanjit Manohar Majhi received his Ph.D. degree in August and M. S. degrees from Seoul National University and his Ph.D.
2017 from Chonbuk National University, South Korea, and degree from Massachusetts Institute of Technology (MIT) in
worked on the synthesis of noble metal nanoparticles and metal electronic materials in 1986, 1988, and 1994, respectively. He
oxide semiconductors to design core@shell nanostructures for was a senior researcher in the Samsung Electronics Co., from
gas sensor applications. Then he was a Postdoctoral fellow at 1994 to 2000. He was a visiting professor at the Department of
King Abdullah University of Science and Technology (KAUST), Chemistry of the Michigan State University, in 2009. His
Kingdom of Saudi Arabia from March 2018-June 2019. research interests include the one-dimensional nanostructures,
Currently, he is working as postdoctoral researcher at the nanosheets, and gas sensors.
Research Institute of Industrial Science at Hanyang university,
Seoul, South Korea since September 2019. His research interest
includes core-shell NPs, metal-organic frameworks (MOFs), 1D
nanostructures and room temperature gas sensors.
Sang Sub Kim joined the Department of Materials Science and

Engineering, Inha University, in 2007 as a full professor. He
received his B.S. degree from Seoul National University and his
Ali Mirzaei received his Ph.D. degree in Materials Science and M.S and Ph.D. degrees from POSTECH in Material Science and
Engineering from Shiraz University in 2016. He was a visiting Engineering in 1987, 1990, and 1994, respectively. He was a
student at Messina University, Italy, in 2015 and from visiting researcher at NIMS, Japan, for 2 years each in 1995 and
2016–2018, he was accepted as postdoctoral fellow at Hanyang 2000. In 2006, he was a visiting professor at University of
University in Seoul. He has author or co-author of more than 110 Alberta, Canada. In 2010, he served as a cooperative professor at
peer-review papers, including 15 review papers. Currently, he is Nagaoka University of Technology, Japan. His research interests
assistant professor of materials science and engineering at Shi include the one-dimensional nanostructures, nanosheets, and
raz university of technology, Iran. He is interested in the syn gas sensors.
thesis and characterization of nanocomposites for gas sensing
applications.
Tae Whan Kim received his Ph.D. from the Department of

Physics, State University of New York at Buffalo, in 1989. He is
the HYU Distinguished Professor in the Department of Elec
tronic Engineering, Hanyang University. His current research
interests include the fabrication of memristive devices, organic
light-emitting devices, nanogenerators, and sensors.
25

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Nano Energy 79 (2021) 105369

Contents lists available at ScienceDirect

Recent advances in energy-saving chemiresistive gas sensors: A review

Ag decorated SnO2 NWs H2S (0.5) 2 mW – 21.2 [33]

sensor consumed only 100 mW of power. At 300 ◦ C, the sensor exhibited

4.4. MOS structure modified with 2D materials

O2 + e− (hν) → O-2(hν) → O–2 (hν), (13)

Hyoun Woo Kim joined the Division of Materials Science and

Sang Sub Kim joined the Department of Materials Science and

Tae Whan Kim received his Ph.D. from the Department of

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