Environmental Pollution 314 (2022) 120219

Contents lists available at ScienceDirect

Environmental Pollution
journal homepage: www.elsevier.com/locate/envpol

Review

A state-of-the-art review on capture and separation of hazardous hydrogen

sulfide (H2S): Recent advances, challenges and outlook☆
Yi Herng Chan a, Serene Sow Mun Lock b, Mee Kee Wong a, Chung Loong Yiin c, d,
Adrian Chun Minh Loy e, Kin Wai Cheah f, Slyvester Yew Wang Chai g, Claudia Li h,
Bing Shen How g, Bridgid Lai Fui Chin i, j, Zhe Phak Chan a, Su Shiung Lam k, l, m, *
a
PETRONAS Research Sdn. Bhd. (PRSB), Lot 3288 & 3289, off Jalan Ayer Itam, Kawasan Institusi Bangi, 43000, Kajang, Selangor, Malaysia
b
CO2 Research Center (CO2RES), Department of Chemical Engineering, Universiti Teknologi PETRONAS, 32610, Seri Iskandar, Malaysia
c
Department of Chemical Engineering and Energy Sustainability, Faculty of Engineering, Universiti Malaysia Sarawak (UNIMAS), 94300, Kota Samarahan, Sarawak,
Malaysia
d
Institute of Sustainable and Renewable Energy (ISuRE), Universiti Malaysia Sarawak (UNIMAS), 94300, Kota Samarahan, Sarawak, Malaysia
e
Chemical Engineering Department, Monash University, 3180, Victoria, Australia
f
School of Computing, Engineering and Digital Technologies, Teesside University, Middlesbrough, TS1 3BX, United Kingdom
g
Biomass Waste-to-Wealth Special Interest Group, Research Centre for Sustainable Technologies, Faculty of Engineering, Computing and Science, Swinburne University of
Technology, Jalan Simpang Tiga, 93350, Kuching, Sarawak, Malaysia
h
Department of Chemical & Biomolecular Engineering, National University of Singapore, 117585, Singapore
i
Department of Chemical and Energy Engineering, Faculty of Engineering and Science, Curtin University Malaysia, CDT 250, 98009, Miri, Sarawak, Malaysia
j
Energy and Environment Research Cluster, Faculty of Engineering and Science, Curtin University Malaysia, CDT 250, 98009, Miri, Sarawak, Malaysia
k
Pyrolysis Technology Research Group, Higher Institution Centre of Excellence (HICoE), Institute of Tropical Aquaculture and Fisheries (AKUATROP), Universiti
Malaysia Terengganu, 21030 Kuala Nerus, Terengganu, Malaysia
l
Henan Province Engineering Research Center for Biomass Value-added Products, School of Forestry, Henan Agricultural University, Zhengzhou, 450002, China
m
Sustainability Cluster, School of Engineering, University of Petroleum & Energy Studies, Dehradun, Uttarakhand, 248007, India

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

Keywords: Hydrogen sulfide (H2S) is a flammable, corrosive and lethal gas even at low concentrations (ppm levels). Hence,
H2S the capture and removal of H2S from various emitting sources (such as oil and gas processing facilities, natural
Capture emissions, sewage treatment plants, landfills and other industrial plants) is necessary to prevent and mitigate its
Removal
adverse effects on human (causing respiratory failure and asphyxiation), environment (creating highly flam­
Performance
Feasibility
mable and explosive environment), and facilities (resulting in corrosion of industrial equipment and pipelines).
In this review, the state-of-the-art technologies for H2S capture and removal are reviewed and discussed. In
particular, the recent technologies for H2S removal such as membrane, adsorption, absorption and membrane
contactor are extensively reviewed. To date, adsorption using metal oxide-based sorbents is by far the most
established technology in commercial scale for the fine removal of H2S, while solvent absorption is also
industrially matured for bulk removal of CO2 and H2S simultaneously. In addition, the strengths, limitations,
technological gaps and way forward for each technology are also outlined. Furthermore, the comparison of
established carbon capture technologies in simultaneous and selective removal of H2S–CO2 is also comprehen­
sively discussed and presented. It was found that the existing carbon capture technologies are not adequate for
the selective removal of H2S from CO2 due to their similar characteristics, and thus extensive research is still
needed in this area.

origin of life on earth since 3.8 billion years ago, serving as organic
1. Introduction product, reactant, proto-enzyme, proto-membrane, and primordial en­
ergy source for the chemolitotrophic organisms (Olson and Straub,
Hydrogen sulfide (H2S) has been playing an important part in the 2016). After the Great Oxidation Event occurred in 2.3 billion years ago,

This paper has been recommended for acceptance by Hocheol Song.

☆

* Corresponding author. Pyrolysis Technology Research Group, Higher Institution Centre of Excellence (HICoE), Institute of Tropical Aquaculture and Fisheries
(AKUATROP), Universiti Malaysia Terengganu, 21030 Kuala Nerus, Terengganu, Malaysia.
E-mail address: lam@umt.edu.my (S.S. Lam).

https://doi.org/10.1016/j.envpol.2022.120219
Received 19 August 2022; Received in revised form 12 September 2022; Accepted 16 September 2022
Available online 20 September 2022
0269-7491/© 2022 Elsevier Ltd. All rights reserved.
Y.H. Chan et al. Environmental Pollution 314 (2022) 120219

Abbreviations MOF Metal organic framework

MSR Microbial sulfate reduction
AAIL Amino acid ionic liquid NCG Non-condensable gas
AC Activated carbon NG Natural gas
AMP 2-amino-2-methyl-1-propanol NMP N-methyl-2-pyrrolidone
BTEX Benzene, Toluene, Ethylbenzene, Xylene NP Nanoparticle
CA Cellulose acetate PDMS Polydimethylsiloxane
CCS Carbon capture and sequestration PEG Polyethylene glycol
CNT Carbon nanotube PEI Polyethylenimine
CTA Cellulose triacetate PEO Polyethylene oxide
DEA Diethanolamine PG Propylene glycol
DES Deep eutectic solvent PP Polypropylene
DFT Density functional theory PPO Polypropylene oxide
DMS Dimethyl sulfide PSf Polysulfone
ED Ethylenediamine PTFE Polytetrafluoroethylene
EG Ethylene glycol PVDF Polyvinylidene fluoride
FFV Fractional free volume PZ Piperazine
GO Graphene oxide SILM Supported ionic liquid membrane
HBA Hydrogen bond acceptor TEA Techno-economic analysis
HBD Hydrogen bond donor TR Thermally rearranged
IL Ionic liquid TRL Technology readiness level
LCA Life cycle assessment TSR Thermochemical sulfate reduction
MDEA Methyl diethanolamine ZIF Zeolitic imidazolate framework
MEA Monoethanolamine

H2S has been implicated to several mass extinction events on earth due
to its toxicity and ozone destruction potential (Kump et al., 2005). It
could be released into the atmosphere from ocean floor by upwelling
and diffusion process when the downward diffusion flux of oxygen with
ability to oxidize H2S from air-sea interface was overcome (Hansen
et al., 1978). With the recent observation on ocean deoxygenation that
happens as an effect of warming earth surface and changing biogeo­
chemical cycles (Tessin et al., 2021), this raises the question of whether
extensive H2S eruption from ocean will occur again (Ward, 2006). Other
than ocean, H2S also occurs naturally in hot springs, volcanoes, water
wells, lakes, petroleum wells, and natural gas (NG) wells. Human eco­
nomic activities either release the naturally occurring H2S through pe­
troleum refining and NG treating, or produce H2S through biogas
production, municipal waste and sewerage. There is a need to capture
and convert the anthropogenic H2S as well as the naturally occurring
H2S when required due to its harmful properties.
H2S is a highly toxic, corrosive, and flammable gas, distinguishable
by a strong pungent ‘rotten egg’ odor. At low concentration (up to 20
ppm), H2S causes tearing of eyes, respiratory problems, fatigue, loss of
appetite, headache, irritability, poor memory, and dizziness. At medium
concentration (up to 150 ppm), it could bring about health effects such
as eye irritation, throat irritation, drowsiness, and loss of smells. At high
concentration (up to 2000 ppm), H2S causes serious damage to eyes,
immediate collapse, and death (OSHA, 2021). Due to its dangers,
exposure limits are set in place to protect workers in which the
permissible exposure limits are 20 ppm (also considered as the general
industry ceiling limit), 50 ppm (general industry peak limit) and 10 ppm
(construction and shipyard 8-h limit) (OSHA, 2021). The National
Institute of Occupational Safety and Health (US) defines 100 ppm as the
IDLH (immediately dangerous to life and health concentration) for H2S
(NIOSH, 1994). In terms of emission control, H2S is not included in US
National Ambient Air Quality Standards, while Malaysia Environmental
Quality Regulations 2014 stipulates that the emission limits of H2S for
lime kilns and chemical/petrochemical industries are 15 mg/m3 (11
ppm) and 7.5 mg/m3 (5 ppm), respectively.
H2S is slightly denser than air, therefore it always accumulates at
poorly ventilated lower ground where H2S poisoning accidents tend to
happen. When in contact with air, H2S is rapidly oxidized into SO2 and
sulfate by radicals and other atmospheric oxidants, hence it has a short
residence time of approximately 15 days in the atmosphere (Ausma and
De Kok, 2019). H2S dissolves slightly in water to form weak acid which
causes corrosion to pipelines. However, H2S could act as corrosion in­
hibitor under certain conditions (such as low H2S concentration of below
0.04 mmol/dm3 and pH value of 3–5) by forming a layer of protective
ferrous sulfide film (Ma et al., 2000). H2S can react with a variety of
metal ions to form insoluble metal sulfide, and this property makes it a
potent poison to catalytic processes employing reduced metals as the
primary active phase (Dunleavy, 2006).
This review is systematically structured into several sections. Firstly,
the source of anthropogenic H2S emission is covered in Section 2. In
Section 3, the recent technological advancement of H2S capture and
removal technologies are extensively reviewed and discussed with
regards to their operation conditions, performance/efficiencies, current
limitations and future outlook. This is followed by the comparison of
feasibility and technology readiness level between simultaneous and
selective H2S-CO2 removal in Section 4, which could serve as important
benchmarks for charting the way forward towards sustainable and
improved industrial operations.
2. H2S emitting sources
H2S is one of the dominant elements of sulfur cycle which can be
generated in the environment anthropogenically through a variety of
industrial practices, degradation of sulfur-containing compounds as well
as anaerobic breakdown of sulfates by bacteria, as shown in Fig. 1.
2.1. Extraction and processing of oil and gas
One of the main H2S emission sources is the oil and gas process in­
dustry through operations such as exploration, extraction, refining,
transportation, etc. The corrosive properties and toxic effects of H2S
pose complications to the performance of oil and gas extraction. King
et al. (2013) stated that almost 60% of the sulfur and SO2 used in the
production of sulfuric acid were supplied from the purification of NG
and refining of petroleum supply. The hydrotreating process in petro­
leum refining, used for the removal of sulfur compounds from crude oil

2
Y.H. Chan et al.
Fig. 1. Interconnected chemical processes of H2S in global sulfur cycle
(Modified with permission from Ref (Rubright et al., 2017). Copyright
2017, Elsevier.).
by H2, leads to the production of H2S. The sulfur compounds are reduced
to H2S through refining processes in desulfurization of petroleum stocks
such as distillation, amine systems, water from knockouts and wash
(Reverberi et al., 2016). In this sense, the water-cooled amine absorber
employed to process hydrogenated compounds would generate
H2S-contaminated wastewater streams. Wastewater is also produced
from the utilization of water at start-up/cooling as well as hydrogena­
tion units’ purged water. In addition, hydrocrackers, fluidized catalytic
crackers and hydro-desulfurization units also generate a substantial
amount of sour water consisting of H2S, NH3, and phenols (Addington
et al., 2011).
H2S can also be emitted to the surrounding environment through
various routes due to its high solubility in oil. These include volatiliza­
tion, tank venting due to alteration in temperature, ineffective air
emission control instruments, generation by sulfur-reducing bacteria in
oil and migration/leaking through poorly plugged wells. H2S may also
be accidently released through potential sources such as equipment
failures, piping ruptures and venting due to extreme changes in pressure.
The principal origins of H2S in the production of hydrocarbons are
aquathermolysis (cyclic steam stimulation, steam-assisted gravity
drainage), microbial sulfate reduction (MSR) (water flooded oil reser­
voirs, ground water wells, conventional sour gas reservoirs) and ther­
mochemical sulfate reduction (TSR) in conventional carbonate
reservoirs. These three intricate chemical reactions can lead to forma­
tion of indigenous and non-indigenous H2S in the production of hy­
drocarbons. It is worthwhile to note that desulfurization of sulfur-
containing oils at the processes of hydrogenation and upgrading will
lead to generation of H2S (Marriott et al., 2016). The disproportionation
of the S–H2O system in TSR will be shifted once it is exposed to extreme
acidic conditions. According to Pirzadeh et al. (2014, 2015), chemical
additives can function as reductant and oxidant for hydraulic fracture
fluids in delaying H2S formation via TSR reactions. It is timely for op­
erators and decision-makers to develop effective monitoring systems
and efficient emission control automations for protecting environment
as well as safeguarding the health and safety of employees and general
population (Papailias and Mavroidis, 2018).
2.2. Natural emissions
There is only a small estimated amount of natural emission of H2S
(4.4 Tg/year) out of the total estimated emission of natural sulfur gas
emission (52 Tg/year) (Ausma and De Kok, 2019; Watts, 2000), while
dimethyl sulfide (DMS) and SO2 make up the majority of this emission
which consists of 24.5 and 23 Tg/year, respectively (Watts, 2000; Carn
et al., 2017). Habeeb et al. (2018) stated that hot springs, volcanoes and
other geothermal sources also release H2S. Anaerobic digestion of
organic materials through sulfate-reducing bacteria often contributes to
3
Environmental Pollution 314 (2022) 120219
the emission of H2S to the environment (Jin and Pei, 2015). The natural
breakdown of organic materials in oxygen-deficient conditions, for
instance hydrocarbon deposits, swamps, undersea vents, volcanoes,
stagnant bodies of water, sulfur springs and well-water, also emits sig­
nificant amount of H2S (Chou et al., 2016).
Another natural H2S emitter is geothermal power plants, in which
geothermal steam consists of different quantities of non-condensable
gases (NCGs), such as H2S and carbon monoxide (CO) which may lead
to health, safety and environmental problems if there is no proper
capture and disposal. There are also other toxic compounds produced
along with H2S when the gases within magma such as F, SO2, CO2, Cl,
CO, N, Ar, H and S blended with H2O and H2 (Rubright et al., 2017). In
recent years, attention has been focused directly to agricultural and
man-made sources of H2S instead of geothermal activity. A NCG stream
and a condensate stream, consisting of CO2, H2S and N2, are produced
when the turbine’s exhaust moves through a condenser. The composi­
tion of H2S in the exhaust NCG from conventional steam turbines in high
enthalpy depends on the type of condenser and the amount of H2S input
into the turbine. According to Chou (2003) and Rubright et al. (2017),
the yearly emission sources from land (53–100 million metric tons of
sulfur) and ocean (27–150 million metric tons of sulfur) are comparable
with each other. Hence, this implies that geothermal emissions represent
a substantial source of environmental H2S.
Interestingly, high emission levels of H2S to the atmosphere from
volcanic eruptions has resulted in diverse mass extinctions throughout
history of the Earth (Knoll et al., 2007). Sulfur is released into the at­
mosphere in the form of H2S and SO2 whenever there is a volcanic
eruption. In this regard, oxidation state of the magma source is generally
reflected based on the ratio of H2S/SO2, whereby it differs remarkably
according to the tectonic setting, type of activity, etc (Hoshyaripour
et al., 2012). Sulfurous gases generally contribute 2–35% of volcanic gas
emissions, which are emitted as H2S and SO2 in the quantity of 1–37
Tg/year and 15–21 Tg/year, respectively (Hoshyaripour et al., 2012;
Halmer et al., 2002). According to Hoshyaripour et al. (2012), the
complexities in detecting H2S spectroscopically in volcanic clouds and
analytically resolving S speciation in high-temperature gases have
resulted in limited data of concurrent examinations and quantifications
of volcanic H2S and SO2. The redox ratio (molar ratio of H2S/SO2) in­
creases with reducing oxygen fugacity and magma temperature, and
with growing pressure. Volcanic vents act as high-temperature reactors,
in which changes in the sulfur speciation could generate new reaction
product through the reaction of volcanic mixtures with atmospheric
gases. Based on recent studies, the reaction rates of volcanic gases at
high temperature of above 500 ◦ C are relatively fast to maintain the
equilibrium of the system. H2S is stable in terms of its kinetic throughout
its short-range transport below 600 ◦ C since there is no structured
change with volcanic plume aging according to H2S/SO2 ratio (Martin
et al., 2009). Nevertheless, the sink for H2S still remains unknown in the
condition of additional air entrainment and high temperatures.
H2S has also been detected in the Black Sea due to the usage of
organic wastes and fertilizers in breeding. Organic wastes and fertilizers
consist of extremely high phosphate and nitrate content leading to the
primary production of algae and subsequently the consumption of dis­
solved O2. The decay of algae then leads to sulfates consumption
through the bacteria and the generation of H2S. Nevertheless, there is no
proof currently showing the correlation between shoaling of the H2S
onset depth and that of O2. Although the stratification of the Black Sea is
assumed to be stable overall, there is a possibility that the accumulated
H2S may penetrate through the oxygenated layer due to geological cir­
cumstances or unsteady climate, which can bring significant conse­
quences to the aquatic life. These processes must be modelled with
quantification of H2S concentration for the purpose of regulating the
situation and further resolving the vitals of the H2S (University of Liège,
2016).
Y.H. Chan et al.
2.3. Sewage treatment facilities, landfills, livestock farms
The wastewater treatment process produces excess activated sludge,
which is an unavoidable by-product. The sludge generated from the
wastewater treatment process contains 80% of the organic content,
whereby 50% of the organic content consists of protein (Cui et al.,
2022). Naturally, the sludge will produce unpleasant smell to the envi­
ronment and have a tendency to decompose. The unpleasant smell is
derived from the H2S and methyl mercaptan (MeSH) originated from the
sewage sludge, resulting in negative effects to human health especially
to the respiratory, digestion, endocrine and nervous system (Han et al.,
2020). The generation of H2S and MeSH are formed from methane
bacteria and reduction bacteria without involving oxygen in the process
(Cui et al., 2022). It was reported that the reduced sulfur content,
particularly the H2S derived from the sewers in Australia (This­
tlethwayte and Goleb, 1972) and wastewater treatment plant in United
States (Devai and DeLaune, 1999), is in the range of 0.3 × 103–13.9 ×
103 and 17–446,900 μg/m3, respectively.
Landfill is also another odor pollution source emitted from the
decomposition of organics in municipal solid waste (Fang et al., 2012). It
has been reported that the landfill odor consists of 100 types of com­
pound (Parker et al., 2002) and around 1% of the gas released from
landfill is H2S (Kim, 2006). According to Kim (2006), the emissions of
gaseous pollutant in the landfill facility often take place at the vented
pipes and landfill surfaces. The degree of decomposition in the landfill
strata varies throughout the different developmental stages of the
landfill facilities (Kim, 2006). The concentration of H2S from young
landfills is ca. 139 ppm (Kim, 2006) and the construction and demolition
debris landfills produce a wide range of concentration between 3 ppm
and 12,000 ppm of H2S (Lee et al., 2006a). In another study by Xu and
Townsend (2014), the H2S emission rates and intensities at construction
and demolition debris landfills increased from morning to afternoon and
were influenced by factors such as H2S concentration, soil moisture and
temperature.
It has been reported that breeding poultry such as pigs and cattles
released high amount of organic sulfur and ammonia content (Melse and
Hol, 2017). Blazy et al. (2015) documented that the organic sulfur
compounds released from such farm were in the range of 0.02–0.07 ppb
which resulted in the compost odor concentration of 6289 OUE/m3. In
addition, the methionine is also included in the poultry feed to increase
the immunity of the poultry, resulting in a release of nitrogenous and
sulfurous poultry excretion (Wang et al., 2021a).
2.4. Other industrial plants (coke oven plants, kraft paper mills)
In the steel industry, the coke oven gas is one of the by-products used
as an energy replacement for NG (de Oliveira Carneiro et al., 2021). Due
to the sulfur content in coal, H2S can be formed. The presence of H2S in
the coke oven gas will lead to negative effects such as pipe and equip­
ment corrosion and also SOx emission via the combustion process taking
place in the boilers and flares (Kazak et al., 2018; Safari and
Vesali-Naseh, 2019). Due to the limited resource of low-sulfur coal, the
industry resorted to using coal with high sulfur content leading to high
H2S in the coke oven gas (Zou et al., 2017).
Other than that, kraft mills are often linked to generation of four
reduced sulfur gases, i.e., H2S, MeSH, dimethyl-sulfide (CH3)2S and
dimethyl-disulfide (CH3)2S2 (Rava et al., 2008). The point source of
reduced sulfur emission sources from the kraft mills are the recovery
furnace, smelt-dissolving tanks, lime kilns, brown-stock washers, evap­
orators, digesters, condensate strippers, recovery system of tall oil,
storage tank for liquor, condensate stripper and oxidation system for
black liquor (O’Connor et al., 2000). Meanwhile, the diffuse source
emission includes clarifiers, thickeners, wastewater treatment system
and on-site landfills (O’Connor et al., 2000).
4
Environmental Pollution 314 (2022) 120219
3. H2S capture/removal technologies
3.1. Membrane
Membrane separation is an established technology in a variety of
industrial processes. Due to its smaller footprint, high modularity, lower
weight (high membrane area per unit module) and the ease of operation
as compared to other technologies such as absorption and adsorption,
H2S (usually along with CO2) removal, is often accomplished cost-
effectively via membrane separation in remote areas and subsea/
offshore (He et al., 2020). However, current research and development
of membrane materials are mostly targeted for CO2 removal rather than
H2S removal (Dalane et al., 2017). This is reflected from a large number
of published review papers to date (Shi et al., 2020; Valappil et al., 2021;
Han and Ho, 2021; Yong and Zhang, 2021), which focused mostly on the
membrane separation of various industrial gases (light hydrocarbons,
CO2, N2, O2 and H2), but H2S separation was not covered, except that
George et al. (2016) and Alqaheem et al. (2017) reported reviews
focusing on the development of polymeric membrane for acid gas (CO2
and H2S) removal.
In essence, membrane separation process employs a physical porous
barrier whereby selective gas transport (permeation) occurs as driven by
the presence of transmembrane pressure. Over the years, a myriad of
membrane materials has been engineered to improve the performance,
efficiency and economy of the separation process, all of which revolving
around optimizing several critical parameters in the context of mem­
brane operations, i.e., permeability, selectivity, chemical and mechan­
ical stability (He, 2018). In this sub-section, recent developments of
various types of membranes for H2S removal are reviewed and discussed
in detail.
Polymeric membranes have been proven as successful dominant
candidates that are widely deployed in industrial H2S separation in
various configurations (Shi et al., 2020). Several polymeric membranes
for CO2 bulk removal, also capable of co-removing H2S, have been put in
commercial operations of NG sweetening and biogas upgrading for
several decades, such as cellulose acetate (CA) based Cynara®/Cameron
(Schlumberger, 2016) and Separex™/UOP (Honeywell, 2011), and
polyimide based MEDAL™/Air Liquide (Air Liquide, 2016). Polymeric
membrane gas separation is typically governed by a fundamental
permeability-selectivity trade-off relationship, in accordance with the
Robeson upper bound which registers the current capabilities of various
polymeric membranes in gas separations (Robeson, 2008). Besides, gas
permeation in polymeric membranes is fundamentally governed by the
solution-diffusion transport mechanism (Sanders et al., 2013). Liu et al.
(2020a, 2020b) demonstrated the opportunities of tapping into the
advantage of controlled plasticization of glassy cellulose triacetate
(CTA) hollow fiber and 6FDA-based polyimide dense film membranes
for NG sweetening. Both studies reported that attractive membrane
performance for H2S removal could be achieved even in the event of
plasticization under harsh feed gas conditions, i.e., high H2S (20 mol%),
hence further offering a margin for performance optimization. In
particular, high H2S permeance of ca. 140 GPU and H2S/CH4 selectivity
of ca. 28 were obtained by CTA hollow fiber membranes at 35 ◦ C and
31.3 bar (Liu et al., 2020a), whereas 6FDA-DAM recorded a perme­
ability of 495 Barrer and H2S/CH4 selectivity of ca. 31 at 35 ◦ C and 46
bar (Liu et al., 2020b). These findings were attributed to the funda­
mental controlling mechanisms of the said membranes with the
H2S/CH4 gas pair (i.e., separation of H2S from CH4), in which perme­
ation of H2S was heavily dominated by sorption-selectivity and nega­
tively influenced by diffusion-selectivity. As such, when plasticization
occurred, the creation of free volume in the membrane enhanced the
sorption of H2S and subsequently H2S/CH4 selectivity, while the
diminished molecular sieving effect of the membrane caused a drop in
CO2/CH4 selectivity, which was found to be strongly relying on
diffusivity-selectivity (Liu et al., 2020b).
Other than the highly selective and diffusion-controlled glassy
Y.H. Chan et al. Environmental Pollution 314 (2022) 120219

polymers, rubbery polymers have also been employed for gas separation
due to their high permeability (George et al., 2016). Rubbery polymers
are flexible at ambient conditions due to their low glass transition
temperatures, and thus the transport across rubbery membranes mainly
relies on solubility (Yampolskii et al., 2014). This would be favorable for
H2S removal from CH4, which is solubility-controlled (Liu et al., 2020b).
Harrigan et al. (2020) reported tunable performance of polyethylene
glycol (PEG)-based membrane by varying the crosslinking density to
manipulate the crystallinity of the polymer. This rigidification strategy
was effective to resist the profound effect of plasticization, while
simultaneously improved the diffusion in a solubility-controlled mem­
brane, resulting in impressive CO2/CH4 and H2S/CH4 selectivities of
>60 and >110, respectively. Besides, polydimethylsiloxane (PDMS) is
one of the rubbery polymers having the largest permeability among all
other polymeric membranes, and thus it has been studied in many works
(Yampolskii et al., 2014). Merkel et al. (2000) conducted fundamental

Table 1
Key findings on H2S separation by membranes.
Membrane Feed gas composition Membrane separation H2S permeability/permeance H2S/CH4 selectivity Reference
conditions
8
High silica CHA-type zeolite 2.13 mol% CO2, 0.3 Temperature: 25 ◦ C 1.70 × 10− mol/m2.s.Pa 3.24 Maghsoudi
membrane mol% H2S, 97.57 mol% Pressure difference: and Soltanieh
CH4 400 kPa (2014)
Permeate pressure:
88 kPa
Cellulose triacetate (CTA) hollow 20 mol% H2S, 5 mol% Temperature: 35, ca. 140 GPU (35 ◦ C, 31.3 bar, ca. 28 (35 ◦ C, 31.3 bar, 100 Liu et al.
fiber membrane CO2, 3 mol% C2H6, 3 50 ◦ C 100 ppm toluene) ppm toluene) (2020a)
mol% C3H8, 100–300 Pressure: 6.9–31.3 bar
ppm toluene, balance
CH4
Dense cellulose triacetate (CTA) 1000 ppm H2S, balance Temperature: 4.7–10.2 Barrer - Lu et al.
membrane N2 22–80 ◦ C (2017)
Pressure: 100–900
kPa gauge
Dense polyimide membranes: 6FDA- (i) 0.5% H2S, 20% CO2, Temperature: 35 ◦ C 207–1087 Barrer (6FDA-DAM); 14–38.7 (6FDA-DAM); Liu et al.
DAM; 6FDA-DAM/DABA (3:2) 79.5% CH4; Pressure: 7–46 bar 22.8–87.4 Barrer (6FDA-DAM/ 18.8–49.1 (6FDA-DAM/ (2020b)
(ii) 5% H2S, 45% CO2, DABA) DABA)
50% CH4;
(iii) 20% H2S, 20% CO2,
60% CH4
Crosslinked telechelic poly (ethylene 3% CO2, 5% H2S, 92% Temperature: 25 ◦ C ca. 0.08–25 Barrer 65–116 Harrigan
glycol) membrane CH4 Pressure: 800 psi et al. (2020)
Vinyl-added poly (norbornene)s (i) 5% H2S, 3% CO2, Temperature: 25 ◦ C ca. 4500–6000 Barrer (ternary ca. 6–45 (ternary gas Lawrence
(VAPNBs) membrane 92% CH4; Pressure: 800 psi gas mixture); ca. 6000–7000 mixture); ca. 9–40 (5- et al. (2020)
(ii) 20% H2S, 10% CO2, Barrer (5-component gas component gas mixture)
10% N2, 3% C2H6, 57% mixture)
CH4
Thermally rearranged (TR) 1000 ppm H2S, balance Temperature: 25, 35, ca. 155–170 Barrer (6FDA-HAB- - Scholes et al.
membranes formed from 6FDA- N2 55, 75 ◦ C DAM); ca. 130–150 Barrer (2017)
HAB-DAM and 6FDA-HAB-DAM- Partial pressure: (6FDA-HAB-DAM-DABA)
DABA 0.2–0.9 kPa
(corresponding to
feed pressure of
200–900 kPa)
Copolyimide membranes: 6FDA- 20 vol% H2S, 10 vol% Temperature: 22 ◦ C 52.7–68.0 Barrer (6FDA-DAM/ 19.7–21.2 (6FDA-DAM/ Yahaya et al.
DAM/6FpDA (1:3); 6FDA-DAM/ CO2, 57–59 vol% CH4, Pressure: 24, 35, 46 6FpDA); 61.7–70 Barrer (6FDA- 6FpDA); 23.4–23.9 (6FDA- (2021)
CARDO (1:3); 6FDA-DAM/ABL-21 1–3 vol% C2H6, 10 vol bar DAM/CARDO); 31.5–32.9 Barrer DAM/CARDO); 15.2–15.9
(1:3); 6FDA-DAM/6FDA-CARDO % N2 (6FDA-DAM/ABL-21); ca. (6FDA-DAM/ABL-21); ca.
(1:1) 115–180 Barrer (6FDA-DAM/ 23–25 (6FDA-DAM/6FDA-
6FDA-CARDO) CARDO)
Amine (butylamine; sec-butylamine; 0.5. 1.2, 2.5% (6000, Temperature: 30 ◦ C (6.2–7.6) × 10− 7 mol/m2.s.Pa 7–8.4 (butylamine); 3.9–4.8 Gilani et al.
dodecylamine; octadecylamine) 12,000, 25,000 ppm) Pressure: 1–5 barg (butylamine); (3.2–4.1) × 10− 7 (sec-butylamine); 5.5–7 (2016)
functionalized carbon nanotube H2S, balance CH4 mol/m2.s.Pa (sec-butylamine); (dodecylamine); 3.5–4.5
(CNT) membranes (4.7–5.7) × 10− 7 mol/m2.s.Pa (octadecylamine)
(dodecylamine); (2.9–3.6) ×
10− 7 mol/m2.s.Pa
(octadecylamine)
Supported ionic liquid membranes H2S in N2 Temperature: ca. 1800–8691 Barrer 19.8–142 (ideal selectivity) Zhang et al.
(SILMs): [bmim][PF6]; [bmim] (corresponding to 30–60 ◦ C (2017)
[BF4]; [bmim][Tf2N]; [bmim] partial pressure of Partial pressure:
[TfO]; [bmim][Ac] supported by 0.1–0.5 bar) 0.1–0.5 bar
PVDF flat sheet membrane
Polyphenylene oxide (PPO) hollow 101, 198, 401, 968, Temperature: 22, ca. 15–73 mol/m2.s.Pa (PPO), ca. Separation factor: 1.34–4.1 Niknejad
fiber, poly (ester urethane) urea 3048, 5008 ppm H2S in 40 ◦ C <5 mol/m2.s.Pa (PEUU) (PPO); 3.25–3.43 (PEUU); et al. (2017)
(PEUU) flat membranes CH4; Real natural gas Pressure: 345, 517, Ideal selectivity: ca. 1.5–7.8
(3360 ppm H2S) 689 kPa (PPO)
Triethylene glycol monoesterified 5% H2S, 45% CO2, 50% Temperature: 35 ◦ C ca. 9.5–20 GPU ca. 12–20 (without PDMS skin Babu et al.
crosslinkable (TEGMC) 6FDA- CH4; 20% H2S, 20% Pressure: 100–700 layer); ca. 20–29 (with PDMS (2018)
DAM/DABA (3:2) polyimide hollow CO2, 60% CH4 psig skin layer)
fiber membranes with/without
polydimethylsiloxane (PDMS)
coating layer

(− ) data are not available.

5
Y.H. Chan et al.
study to evaluate the permeability and solubility of 10 gases in PDMS. It
was found that the permeabilities of hydrocarbon gases (CH4, C2H6 and
C3H8) were an order of magnitude higher than the perfluorinated
counterparts (CF4, C2F6, C3F8) due to high solubility and diffusion co­
efficients of the hydrocarbon gases in hydrocarbon-based PDMS.
Another study was reported by Babu et al. (2018) in which a PDMS
coating layer deposited on the crosslinked 6FDA-DAM/DABA polyimide
hollow fiber membranes further promoted the membrane performance
with superb H2S/CH4 selectivity of 22–29 even at aggressive sour gas
feed conditions, i.e., extremely high H2S concentration of 20% and high
pressure of 500–700 psig. It was hypothesized that the PDMS layer
sealed and moderated the morphological defects of the underneath skin
layer of crosslinked polyimide fibers, without which the performance of
the membrane could aggravate under harsh feed conditions.
In addition, to further enhance the performance of polymeric mem­
branes in H2S separation, various scholars have begun to explore some
Fig. 2. (a) H2S permeability of various polymeric membranes (dotted line to aid in visualization of polymeric membranes which exhibited >200 Barrers); (b)
Permeability-selectivity plot for H2S/CH4 gas pair (dotted line represents H2S/CH4 upper bound reported in 2015) (Reproduced with permission from Ref (George
et al., 2016). Copyright 2016, Elsevier.).
6
Environmental Pollution 314 (2022) 120219
new classes of membrane materials, such as thermally rearranged (TR)
polymeric membranes and supported ionic liquid membranes (SILMs)
(Sanders et al., 2013). Thermal rearrangement assists in enhancing
polymer chain flexibility, thereby increasing the fractional free volume
(FFV) of the membrane, which in turn enhances the gas permeability
while preserving the selectivity (George et al., 2016). Scholes et al.
(2017) evaluated the performance of crosslinked and non-crosslinked
6FDA-HAB-DAM polyimide-based TR membranes and revealed the dif­
ference in H2S transport mechanism across these two membranes. The
crosslinked membrane with higher FFV exhibited solubility-dominated
H2S permeation (ca. 130–150 Barrer) compared to its non-crosslinked
counterpart which showed diffusivity-dominated H2S permeation (ca.
155–170 Barrer). Zhang et al. (2017) studied the performance of various
basic and neutral ionic liquids (ILs) impregnated in the polyvinylidene
fluoride (PVDF) flat sheet membrane support. Among all ILs, basic
1-butyl-3-methylimidazolium acetate ([bmim][Ac]) exhibited superior
Y.H. Chan et al.
H2S permeability of 5279 Barrers, and promising H2S/CH4 ideal selec­
tivity of 142 at 30 ◦ C and transmembrane pressure of 0.1 bar. The au­
thors ascribed the findings to the ability of [bmim][Ac] to chemically
absorb the polar H2S through acid-base complexation and behave as a
carrier for H2S transport (facilitated transport) across the membrane. A
series of membranes and their performance in H2S removal obtained
from recent literature is summarized in Table 1, while Fig. 2 provides an
extensive overview of the capability of various polymeric membranes in
the context of H2S removal.
Overall, a variety of membranes have been assessed for their effi­
ciencies and capabilities in H2S removal, targeted particularly for NG
sweetening. To ensure the membranes are robust enough to operate at
realistic and extreme sour mixed-gas conditions, some of these studies
have evaluated the membrane performance using representative high
H2S concentrations of 5–20% in the gas mixture. The main challenge in
H2S removal using membrane, especially for polymeric membranes, is
the susceptibility to physical aging and plasticization in the presence of
plasticizers (H2S, CO2 and condensable aromatics; benzene, toluene,
ethylbenzene, xylene (BTEX)) and high feed gas pressure (Lu et al.,
2018). While a number of membranes showed promising results, few
have gone beyond the lab and pilot phase for commercial adoption.
Another challenge would be the quest for reliable and stable membrane
in simultaneous removal of H2S and CO2 from NG, as the former is
favored by rubbery polymeric membrane and solubility-controlled,
while the latter is favored by glassy polymeric membrane and
diffusion-controlled. In this regard, specialized membrane design aim­
ing to combine the opposing separation preferences of glassy and rubber
polymers, and hence better tunability of membrane properties, is
imperative and entails further in-depth scrutinization. Hybridization of
molecular design and structural engineering strategies, such as cross­
linking, copolymerizing, polymer blending and side-chain functionali­
zation, could be further explored and combined closely (Sanaeepur
et al., 2019). Furthermore, selective separation of H2S from CO2 might
be required if these acid gases were to be managed, converted or utilized
separately downstream. This could initiate new prospect for the adop­
tion of membrane separation technology, while addressing the current
knowledge gaps related to membrane separation of H2S/CO2. Apart
from that, complementary approach via computational methods
(atomistic and molecular dynamics studies) are also essential in assisting
the scientists to grasp the underlying fundamental knowledge and
establish the membrane’s structure-property relationship, which could
provide experimentalists some useful insights and guidance towards
optimal design (Shamsabadi et al., 2021). Lastly, the ease of membrane
fabrication and suitability of commercial membrane manufacturing
techniques to produce the designed membranes also dictate the feasi­
bility of these membranes to be employed industrially. Hence, it is vital
to include this factor into consideration during membrane design.
3.2. Adsorption
Adsorption is an industrially established technology in the context of
fine removal of H2S (polishing). Generally, the adsorption of gas mole­
cules by solid sorbents is controlled by five stages of mass transport
mechanism, namely external diffusion, film diffusion, pore diffusion,
intraparticle diffusion and surface adhesion (Kudahi et al., 2017).
Several common materials including activated carbons (ACs), zeolites,
metal oxides, metal organic frameworks (MOFs), biochar, ash, meso­
porous silica and composite materials have been studied owing to the
high uptake (removal) capacity, good selectivity, good thermal and
mechanical stability to be employed for large-scale cost-and-energy
efficient H2S removal (Georgiadis et al., 2020; Hassankiadeh and Hal­
lajisani, 2020). The efficiency of H2S removal is highly influenced by the
characteristics and properties of adsorbent (porosity and surface
chemistry), as well as the operating parameters (temperature, relative
humidity, gas hourly space velocity and the concentration of H2S, O2
and other contaminants) (Sitthikhankaew et al., 2014). Recent studies
7
Environmental Pollution 314 (2022) 120219
on H2S capture by adsorption are summarized in Table 2.
Currently, metal oxide adsorbents have been successfully deployed
for H2S capture in industrial scales, such as iron oxide-based and mixed
metal oxide-based adsorbents, SULFATREAT and SELECT FAMILY,
respectively (Schlumberger, 2017), and CuO/ZnO-based and activated
alumina-based adsorbents, PuriStar® and Selexsorb®, respectively
(BASF, 2015). Nonetheless, due to the promising capability of metal
oxides as H2S adsorbents, various research and innovation are still
ongoing to further enhance and exploit their superior performance for
H2S removal. Hassankiadeh and Hallajisani (2020) performed a para­
metric study on H2S adsorption by Molybdenum oxide (MnO2) nano­
particles. It was found that the optimum adsorption capacities of 0.081
and 0.074 g H2S/g adsorbent were achieved at 85 ◦ C, 16 bar, 0.018 m/s
superficial velocity and initial concentration of 43 ppm H2S using
non-spherical and spherical sorbent, respectively. The authors proposed
the use of MnO2 as an effective adsorbent due to its high accessibility
and ease of implementation, despite the lower adsorption capacity as
compared to several other composite nano-sized metal oxides such as
graphite oxide/ZnO, NiO/TiO2, CuO/TiO2 and CoO/TiO2 (Hassankia­
deh and Hallajisani, 2020).
Characterized by high surface areas and porosities, zeolites-based
adsorbents are effective industrial adsorbents and have been actively
researched for their applications in H2S removal. Using magnetite
nanoparticles to modify the pore structure and surface chemistry of the
Y and ZSM-5 zeolite substrates, Jafari et al. (2020) compared the per­
formance of both adsorbents to remove H2S (up to 120 ppm) from air at
relatively high temperatures of 100–300 ◦ C in a pilot system. The doping
of 5% magnetite nanoparticles on Y zeolite enhanced the specific surface
area and meso/micropores, hence resulting in an optimum adsorption
capacity of 69.92 mg/g sorbent. In another study by Jameh et al. (2019),
zeolitic imidazolate framework (ZIF-8), a typical MOF, was functional­
ized by ethylenediamine (ED) and tested for its efficiency in H2S removal
from NG. Compared to unmodified ZIF-8 sorbent, ED-modified ZIF-8
exhibited remarkable improvements in terms of adsorption capacity and
breakthrough time, registering threefold and twofold increase, respec­
tively. Due to the presence of ED functional group in the sorbent sub­
strate, the adsorbate-sorbent interaction was drastically enhanced,
leading to high affinity towards the highly polarizable H2S molecules
(Jameh et al., 2019).
Aside from that, porous carbon-based materials such as ACs and
biochars also make up another class of alternative sorbents due to the
low production costs (as they are derived from waste materials usually)
and greener origins (such as biomass-derived ACs and biochars) of the
precursors. Also, these materials usually contain inherent elements and
structural morphologies that serve as conducive sorption sites. Ahmadi
et al. (2021) synthesized a N–S rich nanoporous carbon from jute thread
waste (a cellulosic biomass) activated by KOH. The resultant adsorbent
possessed high surface area (up to 2580 m2/g) and pore volume (up to
1.50 cm3/g), and exhibited superb H2S adsorption capacities of 19.10,
32.59 and 44.95 mmol/g at 1, 10 and 35 bar, respectively. A comple­
mentary density functional theory (DFT) study revealed that the pres­
ence of pyrrolic-N atoms (negatively charged) on the pores facilitated
the adsorption of H2S through hydrogen bonding, and the presence of
negatively charged S atoms around the pyrrolic-N atoms favored phys­
isorption, subsequently giving rise to excellent cyclic performance of the
material (H2S regeneration efficiency of 84% after 5 cycles) (Ahmadi
et al., 2021). A similar study was reported by Wang and co-workers
(2020a), in which peanut shell-derived AC impregnated with Cu and
activated by KOH was employed to capture H2S in confined space. The
carbonization temperature was optimized for the preparation of the
optimal AC with high surface area of 1523.2 m2/g and optimum
adsorption capacity of 97.63 mg/g. The authors further evaluated and
modelled the adsorption isotherm, kinetic and mechanism of the pro­
cess. It was found that the adsorption isotherm was best modelled by the
Langmuir isotherm model, while the kinetic displayed pseudo first-order
trend and the mechanism was governed by combined intraparticle
Y.H. Chan et al.
Table 2
Key findings on H2S capture by adsorption.
Adsorbent
Maize cob waste (MCW)-derived
activated carbon
d-glucose and d-fructose based
porous carbon adsorbents
Nitrogen-modified activated
carbon supported ZnO
adsorbents
Jute-derived nanoporous carbon
adsorbents
Molybdenum oxide nanoparticle
adsorbents
Zeolitic Imidazolate Framework
(ZIF-8) nanoparticle
adsorbents
Pluronic surfactant F127-
modified biosolid-derived
adsorbents
Y and ZSM-5 zeolite supported
magnetite nanoparticle
adsorbents
Thermal-treated residues:
biochar, biomass ashes and
incinerated sewage sludge
Cu-modified activated carbon
fiber
ZnO/MCM-41 adsorbents
Copper impregnated active
carbon derived from peanut
shell char activated by KOH
Environmental Pollution 314 (2022) 120219
Textural properties Adsorption conditions H2S equilibrium adsorption Breakthrough time Reference
capacity (qH2S) (tbr)
SBET: 8–820 m2/g Temperature: 25 ◦ C 0.25–15.5 mg/g 11–629 s Surra et al. (2019)
Vtotal: 0.02–0.35 Pressure: 1 atm
cm3/g H2S concentration: 1100–1800
Vmicro: 0.01–0.32 ppmv
cm3/g Mass of adsorbent: 0.5 g
Vmeso: 0.01–0.04 Particle size of adsorbent: 1–3
cm3/g mm
Gas flowrate: 400 cm3/min
SBET: 229–3217 m2/g Temperature: room 6.32–25.7 mmol/g 18–68.2 min Nicolae et al.
Vtotal: 0.188–1.692 temperature (2020)
cm3/g Pressure: 1 bar
Vmicro: 0.098–1.203 H2S concentration: 20 ppm
cm3/g Mass of adsorbent: 100 mg
Gas flowrate: 0.2 L/min
SBET: 495.1–815.9 Temperature: 30 ◦ C 24.2–62.5 mg S/g 105–345 min Yang et al. (2019)
m2/g H2S concentration: 600 mg/m3
Vtotal: 0.28–0.45 Gas flowrate: 100 ml/min
cm3/g
Vmicro: 0.15–0.24
cm3/g
SBET: Temperature: 25 ◦ C 6.45–19.10 mmol/g (1 bar), - Ahmadi et al.
1064.92–2579.55 Pressure: 1–35 bar 12.77–32.59 mmol/g (10 bar), (2021)
m2/g H2S concentration: Pure (1–10 16.17–44.95 mmol/g (35 bar)
Vtotal: 0.52–1.5 cm3/ bar), 20:80 vol% H2S/He (35
g bar)
Vmicro: 0.01–0.60 Mass of adsorbent: 1 g
cm3/g
SBET: 48–65 m2/g Temperature: 65–89 ◦ C 0.033–0.081 g S/g 78–85 min (at Hassankiadeh and
Pressure: 10–19 bar optimum adsorption Hallajisani (2020)
H2S concentration: 38–73 ppm condition)
Mass of adsorbent: 1 g
Space velocity: 0.018–0.045 m/
s
SBET: 412–1389 m2/g Temperature: 25 ◦ C ca. 8–55 mmol/g (pure H2S, 10 190–400 s (25 ◦ C, 2 Jameh et al. (2019)
Vtotal: Pressure: 0–10 bar (pure H2S), bar), 44–97 mmol/g (mixed gas) bar)
0.4735–0.8694 cm3/ 2 bar (mixed gas)
g H2S concentration: Pure (0–10
Vmicro: bar), 3/7.3/1/88.8 mol% H2S/
0.2824–0.5185 cm3/ CO2/He/CH4 (2 bar)
g
SBET: 110–180 m2/g Temperature: Room 89.1–221.2 mg/g ca. 120–325 min/g Florent and
Vtotal: 0.197–0.394 temperature Bandosz (2020)
cm3/g H2S concentration: 1000 ppm
Vmicro: 0.055–0.078 Volume of adsorbent: 2 cm3
cm3/g Particle size of adsorbent:
425–600 μm
SBET: 332.55–550.08 Temperature: 100, 200, 300 ◦ C 14.7–69.92 mg/g ca. 120–330 min Jafari et al. (2020)
m2/g H2S concentration: 30, 60, 90,
Vtotal: 0.18–0.30 120 ppm
cm3/g Mass of adsorbent: 500 mg
Gas flowrate: 1 L/min
SBET: 3–919 m2/g Temperature: 25 ◦ C 3.1–171.8 mg/g (2.1–38.3 mg/ - Gasquet et al.
Vmicro: 0.000–0.315 H2S concentration: 1250 ppmv cm3) (2020)
cm3/g Mass of adsorbent: 26.7–168.8
g
Gas flowrate: 1 L/min
SBET: 980.8–1768.9 Temperature: 25–110 ◦ C 22.4–75.9 mg/g - Wang et al. (2021b)
m2/g H2S concentration: 0.46 mg/L
Vtotal: 0.51–0.96 Mass of adsorbent: 0.5 g
cm3/g Weight hourly space velocity
(WHSV): 36,000 mL/(g.h)
SBET: 254–739 m2/g Temperature: 50, 175, 300 ◦ C - 119.4–850 min Hazrati et al. (2014)
Vmeso: 0.14–0.49 H2S concentration: 5000 ppm
cm3/g Space velocity: 3000, 7500,
12,000 h− 1
SBET: 1325.5–1523.2 Temperature: 20 ◦ C 34.41–97.63 mg/g - Wang et al. (2020a)
m2/g Humidity: 60%
Vtotal: 0.611–0.736 H2S concentration: 200–1000
cm3/g ppm
Vmicro: 0.475–0.533
cm3/g
SBET: 39.76–901.58 Temperature: Ambient 0.673–1.831 mg/g 63–68 min (ZnAc2- Zulkefli et al.
m2/g Inlet pressure: 1 barg CAC) (2019)
(continued on next page)
8
Y.H. Chan et al. Environmental Pollution 314 (2022) 120219

Table 2 (continued )
Adsorbent Textural properties Adsorption conditions H2S equilibrium adsorption Breakthrough time Reference
capacity (qH2S) (tbr)

Coconut shell activated carbon Vtotal: 0.294–0.434 H2S concentration: 1000–5000

(CAC) modified by CuSO4,
ZnAc2, KOH, KI, Na2CO3
Supported deep eutectic solvent
(SDES) adsorbent: TAECuCl3
supported on fumed silica (FS)
KOH-modified activated carbon
derived from waste oil fly ash
cm3/g ppm
Vmicro: 0.229–0.330 Mass of adsorbent: 32–155 g
cm3/g GHSV: 212.4–780 h− 1 (1.5–5.5
L/min)
L/D (length/diameter) ratio:
0.5–2.5
SBET: 124.07–132.52 Temperature: 20–60 ◦ C 3.87–14.34 mg/g ca. 40–120 min Mao et al. (2020)
m2/g H2S concentration: 800 ppm
Vtotal: (1231 mg/L)
0.5948–0.6295 cm3/ TAECl:CuCl2 ratio: 0.6:1–1.8:1
g Loading of TAECuCl3 on FS:
5–20 wt%
Mass of adsorbent: 1.0 g
Gas flowrate: 100 ml/min
SBET: 35.24 m2/g Temperature: 1–50 ◦ C 3.5–8.5 mg/g ca. 25–120 min Aslam et al. (2019)
Vmicro: 0.0022 cm3/g Pressure: 1 atm
Gas inlet pressure: 20–50 psig
H2S concentration: 50, 100 ppm
Mass of adsorbent: 1 g
Gas flowrate: 0.2–0.8 L/min

(− ) data are not available.

diffusion and film diffusion. The study also showed good regeneration of
the sorbent, with H2S removal rate of above 90% after 5 adsorption
cycles (Wang et al., 2020a).
Florent and Bandosz (2020) attempted the use of sewage
sludge-derived biosolid incorporated with surfactant for reactive
adsorption of H2S. Pluronic surfactant F127 composed of two poly­
ethylene oxide (PEO) attached to both sides of a polypropylene oxide
(PPO) branch was mixed with the biosolid and pyrolyzed at 950 ◦ C to
produce the resulting adsorbent. The study revealed that addition of
pluronic surfactant F127 significantly increased the carbon content and
mesopore volume of the sorbent, and the subsequent pyrolysis treatment
further developed the micropores, leading to better dispersion of the
catalytic adsorption sites (Ca and Fe oxides) and increased the
pyrrolic-N atoms. The increased dispersion of catalytic adsorption sites
provided enhanced reactive adsorption of H2S, at which adsorption and
catalytic oxidation of H2S to elemental sulfur took place, a typical
mechanism involved in the context of H2S capture and removal using
metal oxide-based adsorbents (Hassankiadeh and Hallajisani, 2020). As
a result, highest H2S breakthrough at a capacity of 221.2 mg H2S/g
sorbent (250% increment compared to that of without surfactant) was
obtained, and it outperformed some of the commercial carbonaceous
sorbents such as S-208 (36 mg/g), Centaur® (176 mg/g) and STIX®
(201 mg/g) (Florent and Bandosz, 2020). Gasquet et al. (2020)
compared the efficiency of several waste-derived sorbents, i.e., biomass
ashes, biochar and incinerated sewage sludge in the removal of H2S from
biogas. Among all the sorbents studied, incinerated sewage sludge was
found to be an ineffective sorbent for H2S due to the lack of porosity and
limited surface for sorption. Although biochar exhibited the highest
adsorption capacity of 171.8 mg/g, its low density translated into low
volumetric adsorption capacity, limiting its scale-up. Biomass ashes
appeared to have the highest volumetric adsorption capacities of
22.2–38.3 mg/cm3 (35.6–78.2 mg/g), due to the combination of good
porosity and presence of mineral oxides which catered the catalysis of
HS− oxidation (Gasquet et al., 2020).
In view of the recent trends of research related to H2S adsorption,
several prospects and future research directions are proposed. First, the
use of waste-derived precursors as the building materials for adsorbents
are gaining research momentum as a greener and cheaper alternative.
Various waste materials, such as biomass (Zulkefli et al., 2019), sewage
sludge (Florent and Bandosz, 2020) and fly ash (Aslam et al., 2019),
have been explored for their potential as H2S sorbents. Upcycling of
these wastes into sorbents would promote circular economy and OPEX
reduction, providing sustainable solutions for large-scale implementa­
tion. Secondly, the incorporation/impregnation of metal or metal oxides
into ACs to enhance the H2S removal efficiency could be another way
forward evident from the rising number of publications (Zhao et al.,
2021). As metal or metal oxides are known to be effective sorbents for
H2S, their incorporation into biomass- or waste-derived sorbents could
enhance the performance of H2S removal as compared to that of pristine
or unmodified materials. Thus, systematic life cycle assessment (LCA)
and techno-economic analysis (TEA) for this class of carbon-based
composite H2S adsorbents, which are currently quite limited in the
literature, should be conducted to evaluate their environmental foot­
prints/impacts and life cycle costs (Kozyatnyk et al., 2020; Nowrouzi
et al., 2021) and compared to those of commercial metal oxide-based
H2S adsorbents. Other than that, DFT or computational chemistry
studies could also be actively pursued to complement the empirical
studies. It is a powerful tool that helps scholars to comprehend the
fundamental relationships between adsorption mechanisms, surface
chemistry of sorption sites and morphology of sorbents (Shen et al.,
2018). This in turn can aid in proper material selection as well as pre­
cursor treatment approach.
3.3. Absorption
Absorption by chemical and physical solvents is among the most
established technology for H2S capture. Either in NG or coal gasification
industry, absorption is predominantly employed to remove sour gas
around the world (Babamohammadi et al., 2015). The gas mixture is
contacted with liquid in a column, in which the H2S will dissolve in the
liquid depending on the solubility of H2S in the solvent. This process
where H2S molecules are physically bound in the solvent is called
physical sorption. H2S loading in physical solvents such as Selexol
(dimethyl ethers of PEG) and Rectisol (methanol) and N-methyl-2-­
pyrrolidone (NMP) is driven by pressure difference and not limited by
reaction stoichiometry. Hence, gas streams with high partial pressure of
H2S is advantageous for physical absorption. Regeneration of solvent
can be achieved by adjustment of pressure and temperature (Wang et al.,
2011).
In chemical absorption, solvent reacts with H2S and this reduces the
H2S species in liquid phase. The increased mass concentration potential
difference between gas and liquid phases induces higher mass transfer
and increases liquid film transfer coefficient (Kohl et al., 1997a). Alka­
nolamine solutions are widely used for H2S scrubbing as the solvent can

9
Y.H. Chan et al. Environmental Pollution 314 (2022) 120219

simultaneously remove CO2 and H2S in refineries. Extensive research regenerations of absorbent (Liu et al., 2021b). The summary of experi­
has been conducted to examine the absorption performance of various mental work on H2S absorption and their findings are given in Table 3.
alkanolamines, such as monoethanolamine (MEA), diethanolamine Being the most matured technology for H2S removal, absorption is a
(DEA), methyl diethanolamine (MDEA), 2-amino-2-methyl-1-propanol reliable technology with proven track records in NG, NH3 and H2 plants.
(AMP) and piperazine (PZ) in the past decades (Saha et al., 1993; Tian Despite the successful application of these chemical solvents, there has
et al., 2019a; Lee et al., 2020; Wong et al., 2016). Proprietary amine been concern on corrosiveness, toxicity and environmental impacts of
processes of low energy demand by ExxonMobil (i.e., FLEXSORB™ SE alkanolamines. Besides, the gas stripping process under high tempera­
and OASE® Sulfexx™) and Shell (i.e., ADIP, Sulfinol) enable selective ture is energy intensive and causes loss of solvent via vaporization and
removal of H2S in the presence of CO2 and is claimed to be commercially thermal degradation (Galán Sánchez et al., 2007; Pal and Banat, 2016).
available (ExxonMobil, 2021; Shell, 2021). The traditional hot potas­ Continuous effort in the scientific community to develop new generation
sium carbonate (K2CO3) process was introduced by Benson and Field, of solvents is apparent. Greener solvents such as amino acid salt, IL and
then later licensed as “UOP Benfield™ Process” by Universal Oil Prod­ DES demonstrated promising potential in tackling the shortcomings of
ucts (UOP) (Benson et al., 1954). The inorganic salt solution process is conventional solvents. The high viscosity of IL and DES must be
further improved by incorporating catalyst to promote absorption and considered as it reduces mass transfer coefficient and increases the en­
corrosion inhibition. CATACARB® is commercially successful with more ergy demand for pumping (Babamohammadi et al., 2015; Alkhatib et al.,
than 150 plants in over 30 countries serving mainly the NH3, H2, NG, 2020). Researchers creatively combine functionality of two or more
and ethylene oxide plants (Smith et al., 2016). K2CO3 is often blended classes of solvent in pursuit of the ideal H2S absorbent formulation. The
with promoters, such as boric acid, various amines and amino acids to
increase its slow rate of reaction (Borhani et al., 2015).
IL has been suggested as alternative to conventional physical and
chemical solvents. The unique characteristics of IL having negligible
vapor pressure, high tunability from cation and anion selection as well
as being environmental benign are gaining attention in diverse appli­
cations (Hallett and Welton, 2011; Cevasco and Chiappe, 2014; Bren­
necke and Maginn, 2001; Chan et al., 2020). Tian et al. (2021)
investigated the absorption efficiency of amino acid ILs (AAIL) tethered
with tertiary amine (i.e., MDEA). Both tetramethylammonium arginine,
[N1111][Arg] and tetramethylammonium glycine, [N1111][Gly]
exhibited excellent H2S removal efficiency of 100%. Absorption rate of
acid gas in the tray tower was enhanced by proton-transfer between
AAIL and MDEA (Tian et al., 2021; Tian et al., 2019b). However, high
cost and complex synthesis of IL is a hindrance for application at larger
scale.
More recently, deep eutectic solvents (DESs) have emerged as an
attractive option to address the issues associated with high production
cost of IL (Aissaoui et al., 2017). The green solvent is known to have
negligible vapor pressure, broad liquid range, high thermal stability,
high solvation capacity, biodegradability, non-flammability, low
toxicity and low cost (Zhang et al., 2012; Hayyan et al., 2013). DES
contains a hydrogen bond acceptor (HBA) and hydrogen bond donor
(HBD) made from Lewis or Brønsted acid and base (Smith et al., 2014).
Interaction between H2S and basic DES does not indicate chemical ab­
sorption. DES functionalized by alkaline, amine or oxidizing compo­
nents shows better absorption and regeneration capability compared to
basic alkaline, amine or oxidizing solutions (Wibowo et al., 2021; Wu
et al., 2019). Wang et al. (2020b) added polyethylenimine (PEI) into
DES synthesized from chlorinated choline with ethylene glycol (EG),
urea, glycerol, and propylene glycol (PG). The PEI/DES/EG mixture
demonstrated excellent H2S removal efficiency of 90% after four
regeneration cycles.
There is a rise of attention on gas absorption by nanofluid. Dispersed
nanoparticles, such as SiO2, Al2O3, graphene oxide (GO) and carbon
nanotube (CNT) are added into solvent such as MEA and DEA (Liu et al.,
2021a; Taheri et al., 2016; Esmaeili-Faraj and Esfahany, 2016). The
three-phase system (gas-liquid-solid) improves mass transfer coefficient
via three mechanisms. First, adsorption of gas in the nanoparticles as­
sists the gas transport within the liquid phase. Nanoparticles loaded with
gas is transported from high to low concentration region, which is also
known as shuttle effect. Collision of nanoparticles and the gas-liquid
interface results in thinner diffusion boundary layer. In addition, the
collision also inhibits bubble coalescence. By keeping the bubbles small,
interfacial area for gas and liquid contact is larger. The three mecha­
nisms are illustrated in Fig. 3. Desulfurization performance of
Fe-MEA-BmimCl solution with inert nanoparticles was examined, where Fig. 3. The schematic diagram of (a) shuttle effect; (b) nanoparticles collision;
0.5% of SiO2 in the oxidizing IL showed promising desulfurization and (c) bubble coalescence inhibition (Reproduced with permission from Ref
performance but the H2S removal efficiency declined after multiple (Kim et al., 2014). Copyright 2014, Elsevier.).

10
Y.H. Chan et al. Environmental Pollution 314 (2022) 120219

Table 3
Key findings on H2S capture by absorption.
Solvent Gas composition Gas-liquid contactor Absorption Absorption Capacity Mass transfer Removal Reference
conditions coefficient efficiency

Yellow phosphorus 1200 mg/m3 H2S in Bubble reactor Temperature: - - 88% Mei et al. (2021)
(0.8–2.4 g/L) + N2 55–80 ◦ C
phosphate rock (8.0 g/L) QG: 300 mL/min
Stirring speed:
600–1400 rpm
Fe + MEA + BmimCl + NP: 1000 mg/m3 H2S in Bubble reactor Temperature: 5 mg H2S/g ca. 1.012 100% Liu et al. (2021a)
SiO2, GO, CNT or Al2O3 N2 80–120 ◦ C absorbent mol/(m2.
(0.05–1%) QL: 200 mL/min kPa.min)
ChCl (0.05 mol) + EG (0.1 1000 mg/m3 H2S in Bubble reactor Temperature: - - 100% Liu et al. (2021b)
mol) + DEA (20%) + NP: N2 30–90 ◦ C
Cu, SiO2, CNT or Al2O3 QL: 200 mL/min
(0.1%–2%)
MDEA (30–50%) + 3000–5000 ppm Tray column Temperature: 0.143 mol H2S/mol - 100% Tian et al. (2021)
[N1111][Arg] H2S in N2 30–50 ◦ C absorbent
(2.5–7.5%) Pressure: 1 atm
QG: 2 L/min
QL: 50 mL/min
MDEA (30–50%) + 3000–5000 ppm Tray column Temperature: 0.092 mol H2S/mol - 100% Tian et al.
[N1111][Gly] H2S in N2 30–50 ◦ C absorbent (2019b)
(2.5–7.5%) Pressure: 1 atm
QG: 2 L/min
QL: 50 mL/min
MDEA (30-50 wt%) + MEA 3000–5000 ppm Tray column Temperature: 0.096 mol H2S/mol - 95% Tian et al. (2019a)
(0–0.75%) H2S in N2 30–50 ◦ C amine
Pressure: 1 atm
QG: 2 L/min
QL: 50 mL/min
NaCl (ca. 0.058%) 1000 ppmv Absorption column Temperature: - 0.073/s ca. 99% Kang et al. (2020)
H2S and NH3 in N2 25 ◦ C
pH: 6–10
QG: 1–6 L/min
QL: 1000 ml/min
MDEA (4.5%) + 50 ppm H2S, 15 vol Stirred tank reactor Temperature: 1.8 × 10− 5 mol H2S/ - - Lee et al. (2020)
PZ, AMP, DETA, TEPA, % CO2 and 35 vol % 30–50 ◦ C mol amine
APA, AB, AP, DAB, DBA, CH4 in N2 Pressure: 1 atm
DEP, PED (0.5%)
Fe-EDTA (0–0.05 M) + 5000 ppm H2S and Countercurrent Temperature: - - 100% Marín et al.
Na2CO3 (4–10 g/L 29.5% CO2 in CH4 absorption column Ambient (2020)
Inorganic Carbon) Pressure:
Ambient
QG: 10–40 ml/
min
QL: 5–30 ml/min
MDEA (0.84–2.94 mol/L) 10,000 ppm H2S and Rotating packed bed Temperature: - - 99.98% Zhan et al. (2020)
PZ (0.12–0.58 mol/L) 30% CO2 in N2 29.8–45 ◦ C
High gravity
factor: 40 − 160
QG: ca. 33.3 L/
min
QL: 210–793.3
ml/min
Modified lye contains 100 ppm H2S in N2 Reactor with QG: 0.3 L/min - - 98% Zhang et al.
Na2CO3 (0–2%) + H2O2 atomising nozzle on a (2020a)
(0–1.2%) + SDBS vibration test bed
(0–0.7%)
PEI (5–30%) + ChCl + Gly, 538–897 ppm H2S in Bubble stirred reactor Temperature: - - 100% Wang et al.
EG, PG, urea N2 30–70 ◦ C (2020b)
QG: 250 mL/min
5
Water + NP: GO Pure H2S Bubble column - - 1.91 × 10− - Esmaeili-Faraj
(0–0.025%), SS (0–0.1%) m/s and Esfahany
(2016)
Chelated iron solution 4000–14,000 ppm Rotating packed bed QG: 2.5–6.7 L/ - - 99.85% Liu et al. (2019)
H2S min
QL: 250–666.67
ml/min
Rotational speed:
400–2400 r/min
Fe3+ (0–0.18 M) + H2O2 200–4000 ppm H2S Bubble stirred reactor Temperature: - - 97% Wang et al.
(0–1.2 M) + Ce3+, Mn2+ in N2 25–75 ◦ C (2019)
(0–0.011 M) QG: 400 mL/min,
Initial pH:
1.02–9.2
(continued on next page)

11
Y.H. Chan et al. Environmental Pollution 314 (2022) 120219

Table 3 (continued )
Solvent Gas composition Gas-liquid contactor Absorption Absorption Capacity Mass transfer Removal Reference
conditions coefficient efficiency

Stirring rate:
0–1000 rpm
Fe3+, Cu2+ (0–0.18 M) + 400–5000 ppm H2S Bubble stirred reactor Temperature: - - 98.9% Wang et al.
H2O2 (0–1.2 M) in N2 25–75 ◦ C (2018a)
pH: 1.12–9.01
QG: 0.1–1.5 L/
min
[BDMAEE][AcO], 99.9% H2S Equilibrium cell with Temperature: 0.950 mol H2S/mol - - Huang et al.
[TMPDA][AcO], magnetic stirrer 25–60 ◦ C absorbent (2017)
[TMEDA][AcO], [BMEE] Pressure: ca. 1.3
[AcO] (40-70 wt%) bar
Fe-EDTA (0.10 mol/L) 22,000 ppm H2S, Absorption column Temperature: - - Bench scale: Maia et al. (2017)
0.3% O2, 14.0% 25 ◦ C 99%; Pilot
CO2, 2.4% N2 in CH4 Pressure: 34.5 scale: 97.84%
kPa
QG: 340 mL/min
Seawater + NaOH + Cl2 17.9–28.7 ppm H2S Fritted bubbler QG: 5–15 L/min, - - 98.40% Boumnijel et al.
(0.5–3 g/L) pH: 9.5–11.5 (2016)
DEA (10%) + 30–50 ppm H2S and Wetted wall column Temperature: 1.14 g H2S absorbed - - Taheri et al.
NP: SiO2, Al2O3 1–3% CO2 in CH4 25 ◦ C by nanofluid/g H2S (2016)
(0.005–0.5%) Pressure: 1.8 psig absorbed by the
QG: 0.56 L/min base fluid
QL: 42 ml/min

(− ) data are not available.

major obstacle of these hybrid solvents is to sustain the absorption

performance of the solvents after cycles of regeneration (Maia et al.,
2017; Liu et al., 2021c). More studies in optimizing the regeneration
technique are of utmost importance to compete against commercialized
process. Another prospective proposal is integrating dispersed nano­
particles to improve gas transport properties. The challenge of using
three-phase absorbent is to retain the stability of nanoparticles after
multiple absorption-regeneration (Liu et al., 2021b). In view of this,
nanofluid for gas treatment will benefit from detailed analysis on the
nanoparticles’ surface morphology and structure changes after repeated
regeneration cycles. To bring the technology to commercialization,
comprehensive investigations including process design, energy effi­
ciency and TEA are vital.

3.4. Membrane contactor

A relatively newer technology uses membrane as gas-liquid con­

tactor for acid gas absorption process. Instead of providing a permeable
barrier to selectively separate gases, the membrane serves as a fixed
interface between gas and liquid streams. A highly porous membrane is
preferable to increase gas flux across the membrane. Hollow fiber
membrane is commonly used, where gas from the shell side diffuses
through the membrane pores and crosses into the tube side, where gas is
absorbed in the liquid. Fig. 4 shows a schematic diagram of a hollow
fiber membrane contactor module in counter-current configuration. As
opposed to the pressure-driven conventional membrane gas separation
unit, membrane contactor is concentration gradient-driven (Hedayat
et al., 2011; Mansourizadeh and Ismail, 2009; Chuah et al., 2020).
Membrane contactor is known to have several advantages over tradi­
tional gas liquid contactor, such as larger surface area per volume,
improved hydrodynamic distribution, no entrainment or foaming and
easy to scale-up. The membrane contactor’s specific surface area
(m2/m3) between gas and liquid phases can be more than 5 times of
typical conventional contactors (Qian et al., 2010; Gabelman and
Hwang, 1999; Klaassen et al., 2005; Rongwong et al., 2012; Belaissaoui
et al., 2016).
Qi and Cussler (1985) were the first to investigate application of
membrane as gas liquid contact device to replace conventional packed
or tray column for acid gas absorption. Ideally membrane pores shall
only contain gas, while liquid absorbent remains in the tube. Liquid
penetrating membrane causes higher mass transfer resistance. The
Fig. 4. Reaction between K2CO3/PL mixed solution with acid gases (H2S and
CO2) in a membrane contactor (Reproduced with permission from Ref (Pan
et al., 2020). Copyright 2020, Elsevier.).
phenomenon is called membrane wetting (Kreulen et al., 1993; Bazhe­
nov and Lyubimova, 2016; Lu et al., 2008). Hence, hydrophobic mem­
brane is the better choice to mitigate liquid drops formation in
membrane pores. The pressure control of gas and liquid is also crucial in
maintaining the gas-liquid interface at membrane pore mouth. Howev­
er, aqueous solutions of organic solvent (especially alkanolamines) can
infiltrate the membrane pores and lead to partial wetting (Wang et al.,
2005). The low surface tension of most absorbents increases the ten­
dency of wetting, especially after prolonged operation (Wiheeb et al.,
2013). Combination of membrane with high surface energy and absor­
bent with high surface tension was found to resist pore wicking. Mem­
brane surface energy is generally affected by surface pore size and
porosity (Mosadegh-Sedghi et al., 2014). Materials such as poly­
propylene (PP), polytetrafluoroethylene (PTFE), PVDF, polysulfone
(PSf) and polyethersulfone are widely tested for gas absorption appli­
cations (Bazhenov and Lyubimova, 2016; Lu et al., 2008).
Aside from high surface tension, other favorable features of utilizing
absorbents in membrane system are similar with the benefits of using

12
Y.H. Chan et al.
solvent in absorption technique, such as high equilibrium solubility, fast
reactivity, low regeneration energy and low viscosity. Alkanolamine and
alkaline based salt solutions are widely researched. Applying the
concept of liquid-liquid extraction, Agrahari et al. (2013) examined
effectiveness of PP hollow fiber membrane contactors in degasification
of H2S from wastewater using MEA. Diffusion of gas molecules in the
pore and adsorption-desorption on membrane wall were modelled to
elucidate the mechanism of H2S removal. Considering that CO2 usually
co-exists with H2S in the gas stream, such as NG, biogas and industrial
effluent gas, numerous studies on simultaneous removal of H2S and CO2
were carried out. Jin et al. (2017) found that H2S absorption flux
decreased when CO2 concentration increased. A stability test conducted
for 90 min showed that H2S absorption flux remained the same despite
partial wetting of the PVDF membrane. Separation of high concentration
of H2S in mixed CO2 and CH4 gas was investigated up to 50 bar of
pressure. The study showed that the liquid phase mass transfer resis­
tance was dominant at low pressures while overall mass transfer coef­
ficient was dependent on the gas phase mass transfer resistance at high
pressure (Marzouk et al., 2010). Table 4 summarizes the treatment
performance of various membrane contactors using different
absorbents.
The most discussed challenge of absorption via microporous mem­
brane is the penetration of liquid absorbent resulting in gradual wetting
of membrane pores, which significantly increases the mass transfer
resistance (Wang et al., 2005; Mavroudi et al., 2006; Keshavarz et al.,
2008). The phenomenon is irreversible as the strong capillary force will
keep the liquid inside the pores. One of the suggested solutions is
incorporating a thin and non-porous coating onto the porous membrane
surface to hinder liquid permeation. However, the coating layer allows
water vapor to permeate and condense within the porous substructure,
leading to decline in gas flux (Scholes et al., 2015). The additional
resistance on a thin film composite membrane also affects membrane
performance (Simioni et al., 2011). Another similar approach to ensure
membrane pores to be entirely filled with gas was tested using a
nonporous dense polymeric membrane. The nonporous membrane not
only allowed stable gas-liquid interface, but also showed improved
selectivity for H2S over CO2 and CH4 through solution diffusion mech­
anism (Tilahun et al., 2018a; Tilahun et al., 2018b). Membrane with
smaller mean pore size and lower effective surface porosity could also be
considered to prevent the wetting problem. Nevertheless, it is important
to determine the optimized pore size and its distribution to ensure gas
mass transfer is not compromised (Pang et al., 2020).
Numerous studies dedicated to polymeric membrane contactor
showed positive outcomes as gas-liquid contactor for H2S removal. The
drawback of this material is that it lacks thermal and chemical stability
for industrial application at extreme conditions. To maintain membrane
performance and economy of the gas separation operation under high
temperature, some researchers applied inorganic material such as zir­
conia (ZrO2), silica (SiO2), alumina (Al2O3), and titania (TiO2) to
fabricate membrane (Koonaphapdeelert and Li, 2006; Yu et al., 2015).
The ceramic membrane suffered from inferior gas flux due to the hy­
drophilic nature of the material which was highly susceptible to mem­
brane wetting (Picard et al., 2001). Effort in hydrophobic modification
of conventional ceramic membrane to alleviate absorbent intrusion will
be a huge step forward in terms of technical viability (Yu et al., 2015;
Abdulhameed et al., 2017; Zhang et al., 2021). Coupled with its superior
mechanical strength, high resistance to chemical, thermal and corro­
sion, ceramic membrane could be a desired choice of membrane con­
tactor. The general pros and cons of each H2S capture/removal
technology is summarized in Table 5.
4. Comparison of feasibility and technology readiness level
between simultaneous and selective H2S–CO2 removal
Removal and capture of H2S is an important aspect to be given
consideration since there are a lot of evidence that H2S can accumulate
13
Environmental Pollution 314 (2022) 120219
in the atmosphere to be captured by the moisture for acid rain forma­
tion, which ultimately contributes to terrestrial and aquatic acidification
(Plens et al., 2015). Therefore, the availability and development of H2S
removal technologies play significant roles in assisting industries to
comply with the outlined environmental regulations and safety limit.
Considering that both acid gases, e.g., CO2 and H2S, coexist together in
majority of the emission sources (Georgiadis et al., 2020), evaluation of
the feasibility of the chemical processes can be majorly divided into (1)
simultaneous CO2 and H2S removal and (2) selective H2S–CO2 removal.
Technology readiness level (TRL) and comparison between the two
types of separation have been summarized in Table 6.
If H2S is merely aimed to be removed from the streams, the process is
advantageous from feasibility aspect since most of the carbon capture
and sequestration (CCS) processes with high TRL, e.g., absorption,
polymeric membrane and adsorption, can be employed to achieve the
objective while removing carbon dioxide (CO2) simultaneously. This is
because H2S and CO2 have similar attributes, such as being acidic in
nature and are electron acceptors, which can be effectively removed
using the same established technology since both exhibit comparable
affinity with the developed materials or processes (Georgiadis et al.,
2020). According to a recent analysis conducted by Department of En­
ergy, the approximate cost of CCS technology is at $58.30 per metric ton
of CO2 captured, and is in the realm of further decrement with progress
and advancement in research and development (James et al., 2019). On
the other hand, the cost per metric ton of H2S removal is comparatively
higher due to its minute amount found in the resources (Huertas et al.,
2020). In addition, the technologies for H2S removal are also accom­
panied with wider ranges of capital and operating expenses, which are
dependent upon maturity of the processes (Huertas et al., 2020). Hence,
the simultaneous removal of CO2 and H2S can be achieved using the
existing CCS technology to optimize cost if the appropriate process
design, material selection and operating conditions are to be selected.
Nonetheless, it is important to take note that CO2 and H2S inherit
competitive transport behaviour, which contributes to the negative ef­
fect of CO2 towards H2S removal and vice versa (Georgiadis et al., 2020).
In this context, this causes the reduction in removal efficiency, which
may result in offset of CO2 and H2S composition from the environmen­
tally regulated permissible limit and increase the ultimate separation
cost. In addition, the presence of CO2 complicates the design of suitable
materials and operating parameters for H2S removal due to their
co-existence in bulkier concentrations and its more acidic characteristic
(Georgiadis et al., 2020). Considering the wide range of H2S concen­
trations in different NG reservoirs, this necessitates interrogations using
mixed gas of varying compositions at the experimental scale to elucidate
the competitive behaviour prior to drawing precise decision for TEA and
upscaling at process industry.
From Table 6, it is seen that absorption is the most popular tech­
nology with highest TRL for simultaneous removal of CO2 and H2S,
which can be achieved using amine, alkaline salt and physical solvents.
Although this process has achieved sufficient commercial application,
continuous research and development works have been undertaken to
propose novel solvent blends and ILs to circumvent operational and
economic issues of the absorption process, which include corrosiveness,
degradation, large footprint and energy consumption that contribute to
high capital and operational cost at present stage (Oko et al., 2017).
With regards to membrane separation, polymeric type is most widely
used for commercial application in CO2 and H2S removal with advan­
tages of smaller capital and operating expenses as compared to other
materials and absorption process at the expense of lower product purity.
It has been reported that merely USD 20/m2 of polymeric membrane
active area is required in comparison to inorganic membrane module
that costs as high as USD 3000/m2 (Vu et al., 2003). Membrane con­
tactor that combines both polymeric membrane and solvent as one
intensified separation technology is at the edge of pilot scale testing to
exploit the benefits of the process in order to achieve more cost-effective
separation (Hafeez et al., 2021). On the other hand, mixed matrix
Y.H. Chan et al. Environmental Pollution 314 (2022) 120219

Table 4
Key findings on H2S capture by membrane contactor.
Membrane Membrane Absorbents Gas composition Test conditions Transport Removal H2S/CO2 Reference
material properties properties efficiency selectivity

PP Porosity: 0.25 0.5 M MDEA 5000–25,000 ppm Temperature: KH2S: 0.0223 mol/ ca. 100% 82.7a Mirfendereski
Surface area: 1.4 H2S and 4–20% 25 ◦ C m2.s.atm et al. (2019)
m2 CO2 in CH4 Pressure: 0.5
Surface/volume: bar
9333.3 m2/m3 G/L: 144–960
PDMS Surface area: 1 M NaOH + 0.0115 M 10,000 ppm H2S Temperature: - 100% 4b Tilahun et al.
0.092 m2 K2HPO4 + 0.0075 M and 39% CO2 in 30 ◦ C (2018a)
Thicknesses: 1, 1.5 NH4Cl + 0.001 M CH4 Pressure: 1.05
and 2 mm MgCl2⋅6H2O bar
pH: 7–10
6
PDMS Surface area: 1 M NaOH 10,000 ppm H2S Temperature: KH2S: 6.91 × 10− 99.8% 2.52b Tilahun et al.
0.0659 m2 and 39% CO2 in 10–45 ◦ C m/s (2017)
CH4 Pressure: 1 bar Gas flux: 1.19 ×
pH: 7–10 10− 6 mol/m2.s
QG: 9–35 ml/
min
PVDF Pore size: 0.2 μm 0.025–0.1 M MEA; 300–900 ppm H2S, Temperature: KH2S: 0.0064 m/s - - Jin et al. (2017)
Porosity 0.7 0.025–0.1 M K2CO3; 30–50% CO2 in 25 ◦ C Gas flux: 2.9 ×
0.025–0.1 M KOH; CH4 Pressure: 1–4 10− 6 mol/m2.s
0.025–0.1 M PS bar
pH: 7–10
QG: 300 ml/
min
QL: 40–140 ml/
min
PP Fiber length: 0.16 0.5 M MEA 300–1600 ppm Feed pH: 4 - 98% - Agrahari et al.
m H2S in water Qfeed: 200–400 (2013)
Packing fraction: ml/min
0.435 Qabsorbent:
Pore size: 30 nm 1000 ml/min
Porosity: 0.4
Surface area: 1.4
m2
PTFE, PFA Packing fraction: 0.1–2.0 M NaOH; 0.5 20,000 ppm H2S Temperature: KH2S: 1.96 × 10− 6 - - Marzouk et al.
0.551 (PTFE); M MEA; 0.5 M DEA; and 5% CO2 in CH4 22 ◦ C m/s (PTFE); 2.5 × (2012)
0.324 (PFA) 0.5 M DETA Pressure: 1–50 10− 5 m/s (PFA)
Porosity: 0.181 bar H2S flux: 1.17 ×
(PTFE); 0.568 QG: 600–1000 10− 4 mol/m2.s
(PFA) mL/min (PTFE); 1 × 10− 3
QL: 10–25 mL/ mol/m2.s (PFA)
min
3
PVDF Packing fraction: 0.125–1 M MEA 250–1000 ppm QG: 400–600 KH2S:: 24.3 × 10− 83% - Rongwong et al.
capillary 0.59 H2S and 20–40% mL/min mol/m2.s.atm (2012)
membrane Pore size: 0.2 m CO2 in CH4 vL: H2S flux: 2.15 ×
Porosity:0.7 0.019–0.076 10− 6 mol/m2.s
Surface area: m/s
0.084 m2
PTFE - 0.1–2 M NaOH; 0.1–2 2% H2S and 5% Pressure: 1–50 H2S flux: 1.67 × 100% - Marzouk et al.
M MEA; 0.5 M DEA; CO2 in CH4 bar 10− 4 mol/m2.s (2010)
0.5 M TETA QG: 1000 ml/
min
QL: 10–50 ml/
min
4
PSf, PVDF Surface area: 0.84–2 M MDEA + 1 1100–3100 ppm Temperature: KH2S: 2.63 × 10− 92.8% 28.5a Hedayat et al.
0.0229 m2 (PSf); M MEA; DEA H2S and 20–40% 25–45 ◦ C m/s (2011)
0.0222 m2 (PVDF) CO2 in CH4 QG: 400–600
ml/min
QL: 50–325 ml/
min
3
PP Fiber length: 20 0–2.5 M NaOH 25–2010 ppm H2S pH: 7-13 KH2S: 2.54 × 10− 96% - Jefferson et al.
cm in synthetic air (N2 QG: 850–5000 m/s (2005)
Packing fraction: + O2) ml/min
0.204 QL: 50–650 ml/
Pore size: 0.6 μm min
Surface/volume: G/L: 1–50
2400 m2/m3
PVDF Fiber length: 0.4 m 2 M Na2CO3 1000 ppm H2S and Pressure: KH2S: 0.016 m/s 100% 293a Wang et al.
Packing fraction: 5–23% CO2 in N2 0.2–0.6 bar (2004)
0.36 G/L: 250–1625
Surface/volume:
2506.6 m2/m3

(− ) data are not available.

a
H2S selectivity is defined by ratio of overall mass transfer coefficients of H2S over CO2 (KH2S/KCO2).
b
H2S selectivity is defined by H2S over CO2 concentrations in the liquid phase to that in the gas phase.

14
Y.H. Chan et al. Environmental Pollution 314 (2022) 120219

Table 5 the most common and mature processes for capture of acid gases (e.g.,
Comparison of advantages and disadvantages of H2S capture/removal CO2 and H2S), developing H2S selective amine solvent will be a major
technologies. concern to be overcome for application in H2S utilization route due to
Technology Advantages Disadvantages affinity of most solvents to both CO2 and H2S. Among the chemical
Membrane • Modular configurations, large • Most polymeric membranes
processes, only generic DIPA and MDEA seem to be commonly adopted
surface area per unit volume are limited by the for H2S selective absorption to date (Kohl et al., 1997b). However, the
(lower weight). permeability-selectivity disadvantages of DIPA and MDEA of inheriting higher solvent cost and
• Lesser footprint and easy to trade-off. lower comparative reactivity as compared to conventional amine urge
operate, hence suitable for • Multi-stage design/
ongoing work to propose new physico-chemical solvent, such as
remote or offshore configuration is needed for
applications. fine separation and high- Sulfinol-M, to increase H2S/CO2 selectivity at lower plant cost since it
purity products. operates based on smaller recirculation rate and equipment (Guo et al.,
Adsorption • Commercially established • Might require large footprint, 2005), and in the verge of further improvement via continuing research
and matured technology for hence not suitable for remote and development of new blends and ILs with superior separation per­
fine removal of H2S or offshore applications.
(polishing). • Used sorbent resulting in
formance (Babamohammadi et al., 2015).
• Large surface area and toxic waste generation and With regards to membrane separation, although there has been
porosity facilitating excellent might lead to health and emerging effort to propose novel H2S selective membrane in order to
mass transport, leading to environmental issues. achieve this new avenue, the number of works is still limited and merely
high removal capacity.
at experimental scale investigation stage, while their potential for
Absorption • Commercially established • Corrosiveness, toxicity and
and matured technology for environmental impacts of commercial application has not been resolved to date. In addition, the
bulk removal of H2S. alkanolamines. presence of H2S has been reported to exhibit negative effect on the
• Meets stringent H2S • Solvent regeneration under membrane selective performance, which further complicates the
emissions targets and suitable high temperature is energy breakthrough of developing membrane technology with sufficient H2S/
for tail gas treating. intensive and causes loss of
CO2 selectivity and economic feasibility in commercial application
solvent via vaporization and
thermal degradation. (Nemestóthy et al., 2020). With respect to adsorbent, it is seen from
Membrane • Higher surface area per unit • Additional resistance due to Table 6 that several materials based on iron oxide and molecular sieves
contactor volume and smaller footprint. membrane. have been commercialized for industrial application with superior per­
• No entrainment and foaming. • Membrane wetting, thermal
formance in terms of H2S removal efficiency even at low concentrations
and chemical degradation of
membrane material affect and temperatures (Georgiadis et al., 2020). This finding proves that
performance stability for adsorption process has sufficient economic feasibility, which is compa­
long operation. rable to absorption, for selective H2S/CO2 separation. Nevertheless, in a
similar manner, adsorption is also still ongoing thorough investigation
in the field, especially in the area of uncovering new generation or
membrane that incorporates inorganic material (which is deduced to be
modified adsorbents to achieve higher H2S removal efficiency with full
inappropriate as a standalone separation technology due to its costly
regeneration capabilities. Nonetheless, it has been found to provide a
nature) within polymer structure is able to enhance performance of CO2
clear advantage in terms of a high H2S removal efficiency even at very
and H2S removal (Hafeez et al., 2021). Although this shed light on
low concentrations, which enhances the feasibility of this application.
improvement of membrane techno-economic feasibility in commercial
Lastly, for cryogenic distillation, it has to be properly customized in
application, the status is merely at laboratory interrogation while po­
order to achieve the selective H2S/CO2 separation and hence is less
tential for commercial application in terms of economic feasibility has
commonly practiced in industry as compared to other processes due to
not yet been fully elucidated to date.
its cumbersomeness and higher cost.
Adsorption process is also commercialized for certain materials
In short, it can be seen that for simultaneous CO2–H2S and selective
typically from molecular sieves family for removal of CO2 and H2S but
CO2/H2S removal, respectively, absorption remains as the dominating
limited to feed application at low to medium concentration range only,
technology with the highest TRL for recovery of highly contaminated
which has been attributed to lower sorption capability and selectivity
feed stream while adsorption is commercially used for separation of
depending upon the material selection (Yu et al., 2012). This reduces its
contaminants with low concentration. Nonetheless, these process tech­
economic competitiveness with other separation processes of compara­
nologies are associated with intensive energy requirements for the
ble TRL. Hence, active research is ongoing to uncover new generation of
regeneration of solvent and adsorbent (Elfving et al., 2021). The high
composite or functionalized materials to achieve higher CO2 and H2S
regeneration enthalpy is particularly valid for absorption process owing
removal capability (Yu et al., 2012). Viewing from cryogenic distillation
to the strong chemical interaction between the gas molecules and sol­
point of view, it is used for very sour gas that enables re-injection in
vent, and tremendously high boiling point of the chemical itself.
wells. Although the process has been commercialized, it requires addi­
Emerging effort has been realized to elucidate new generation materials
tional compression and cooling arranged in stages for feed gas prepa­
that are cost effective, efficient, easy to synthesize and regenerate, such
ration, which necessitates high capital cost and energy requirement.
as novel solvent blends, ILs and composite adsorbents (Feng et al.,
Refrigeration cooling to extremely low negative temperature is involved
2023). Another strategy is to propose hybrid or intensified process, such
in the process, which confined the application to probably only suitable
as membrane contactor, that incorporates supplementary technology
for industry with production of liquid CO2 ready for transportation, e.g.,
with relatively lower energy consumption within conventional separa­
liquified natural gas (LNG) to enhance techno-economic feasibility of
tion process in order to reduce the load. Innovations that integrate H2S
the technology (Ghasem et al., 2020).
capture and conversion to higher value-added applications are the way
Nonetheless, the similar characteristics of CO2 and H2S become a
forward to promote circular economy, such as H2S oxidation over
drawback in application in which selective H2S/CO2 separation is
carbon-based catalysts could be employed for the direct production of
required, such as in CO2 and H2S utilization routes that require separate
energy storage materials (Sun et al., 2022). Nonetheless, majority of
highly purified streams for high conversion into targeted value-added
these efforts are mostly confined to research and development phase at
products, which is typically complicated in application that has CO2 in
the laboratory scale, while the actual interrogation and implementation
abundance (Georgiadis et al., 2020). Therefore, not all available CCS
for industrial application remains unresolved. This necessitates more
technologies can be used to achieve the selective H2S/CO2 separation.
scale-up study to reaffirm energy efficiency and feasibility of these new
Although absorption-based technologies have been regarded as one of
processes in actual industry applications.

15
Y.H. Chan et al.
Table 6
Technology readiness level (TRL) and comparison between simultaneous CO2 and H2S and selective H2S–CO2 removal.
Technology
Amine absorption (Kohl
et al., 1997a; Ibrahim
et al., 2014)
Alkaline salt absorption
(Smith et al., 2016)
Physical absorption (Ma
et al., 2021; Burr and
Lyddon, 2008)
Physico-chemical absorption
(Kohl et al., 1997b)
Ionic liquid absorption
(Zhang et al., 2020b;
Huang et al., 2014; Wang
et al., 2018b; Wang et al.,
2018c)
Polymeric membrane (Baker
and Lokhandwala, 2008;
Shah et al., 2017)
Inorganic membrane
(Maghsoudi and Soltanieh,
2014; Makertihartha et al.,
2020; Sedigh et al., 1998)
Membrane contactor
(Hedayat et al., 2011;
Wang et al., 2004; Meyer
and Leppin, 2013)
Hybrid membrane (Liu et al.,
2018; Ahmad et al., 2020;
Lee et al., 2006b)
Pressure/temperature swing
adsorption using pristine
material (Georgiadis et al.,
2020; Huang et al., 2019;
Peluso et al., 2019; Liu
et al., 2020c)
Pressure/temperature swing
adsorption using
composite (Georgiadis
et al., 2020; Huang et al.,
2019; Peluso et al., 2019;
Liu et al., 2020c)
Cryogenic distillation (Shah
et al., 2017; Holmes and
Ryan, 1982)
(− ) data are not available.
5. Conclusions
Efficient capture of H2S is vital to prevent disastrous effects upon
exposure to human, environment and facilities. To date, H2S capture and
removal technologies have been quite established in commercial scales.
Environmental Pollution 314 (2022) 120219
Simultaneous H2S–CO2 Removal Selective H2S–CO2 Removal
TRL Chemical/Material/Unit Commercial Application/ TRL Chemical/Material/Unit Commercial
Manufacturer/Vendor Application/
Manufacturer/
Vendor
9 Monoethanolamine (MEA), BASF, Huntsman, 9 Diisopropanolamine (DIPA) Generic Shell ADIP-
Diethanolamine (DEA), Honeywell UOP, Dow ULTRA
Diglycolamine (DGA), Activated MDEA BASF, Huntsman,
Methyldiethanolamine (MDEA) Honeywell UOP,
Dow, Shell
9 Potassium carbonate (K2CO3) Honeywell UOP Benfield, 6–9 Potassium Carbonate (K2CO3) with ExxonMobil
Eickmeyer & Associates hindered amine activator FLEXSORB SE
Catacarb
Potassium carbonate (K2CO3) with ExxonMobil FLEXSORB PS
hindered amine activator
9 Polypropylene Carbonate (PPC) Fluor Solvent 6–9 Dimethyl Ether (DME) of Polyethylene Honeywell UOP
Glycol (PG) Selexol
Methanol (CH3OH) Linde and Lurgi Rectisol N-Methyl-2-Pyrrolidone (NMP) Linde and Lurgi
Purisol
9 Mixture of DIPA with sulfolane Shell Sulfinol-D 9 Mixture of MDEA with sulfolane Shell Sulfinol-M
(C4H8O2S) and water (C4H8O2S) and water
2–3 Azole-based protic ionic liquids Research and development 2–3 Protic ionic liquids, Alkaline Research and
only functionality ionic liquids, Pyridinium- development only
based ionic liquids
6–9 Cellulose triacetate (CTA) Cameron CYNARA 6–9 Polyether ether ketone (PEEK) ALaS Porogen
PEEK-Sep
Cellulose acetate (CA) Honeywell UOP Separex 2–3 Rubbery membrane, e.g., Research and
Polyimide Air Liquide Advanced Polydimethylsiloxane (PDMS), Poly development only
Separations (ALaS) (ethylene glycol) (PEG), Polyether-
MEDAL block-amide (PEBAX), substituted
Polysulfone Air Product PRISM Polyphosphazenes (PPZ), Poly
Tetrabromo-bisphenol A GENERON (vinylbenzyltrimethyl ammonium
Polycarbonate (TBBPA PC) fluoride) (PVBTAF)
2–3 Ceramic based Research and development - - -
only
1 Carbon based (e.g., graphene (Lei Formulation of basic
et al., 2014), carbon molecular principle only
sieve (CMS)
6 PEEK/DEA Gas Technology Institute 2–3 Polyvinylidene fluoride (PVDF)/Sodium Research and
(GTI) and PoroGen Carbonate (Na2CO3) PVDF and PSF/ development only
Corporation lean MDEA
2–3 Metal-organic-frameworks Research and development 2–3 Supported ionic liquid membranes Research and
(MOFs)/polyimide mixed matrix only (SILM) development only
membrane
9 Molecular sieves-based materials BASF OASE – Gas Treating 9 Iron oxide-based materials Schlumberger
Excellence purple SULFATREAT
Molecular sieves-based materials BASF OASE – Gas
Treating
Excellence yellow
3–7 Pristine metal oxide, biochar, Range from concept 2–3 Modified/functionalized/new Research and
activated carbon (e.g., Desorex validation at the research generation metal oxide, biochar, development only
K43) impregnated with metal and development phase to activated carbon, zeolite, MOFs-based
oxide, zeolite, MOFs-based commercial transition materials
materials depending upon the
material
2–3 Metal oxide/mesoporous silica, Research and development 2–3 Metal oxide/mesoporous silica, metal Research and
metal oxide/activated carbon, only oxide/activated carbon, metal development only
metal hydroxide/activated carbon hydroxide/activated carbon
7–8 Involves classical amine solvent TFE Company and Institut 7–8 Only remove CO2; a dedicated process KOCH Process
downstream to the distillation Français du Pétrole for H2S selective removal have to be Systems or Ryan
column (IFP) Engineering provided upstream of the cryogenic Holmes process
Solutions SPREX process fractionation if required
However, there is still a lot of margins for improvements and optimi­
zation of these processes in the quest for further reduction in technology
costs and enhancement in separation performance. Adsorption using
metal oxide-based sorbents is by far the most successful technology in
commercial adoption for H2S fine removal (H2S in ppm levels), while
16
Y.H. Chan et al.
membrane separation, absorption and membrane contactor are also
established in commercial scales mainly for acid gas bulk removal (H2S
in mol% levels) from natural gas. The removal of H2S by membrane and
absorption has been dominated by polymeric membranes and alkanol­
amine solvents, respectively. Research efforts are still on-going to
further enhance the separation efficiency of H2S by developing effective
and novel materials and solvents, through techniques such as func­
tionalization and molecular design/grafting. Greener and cost-effective
materials and solvents are also the key to improve current H2S separa­
tion performance and should be encompassed in future research. While
H2S can be captured simultaneously with CO2 efficiently using estab­
lished high TRL carbon capture technologies, the selective removal of
H2S from CO2 still demands extensive in-depth research. This would
enable the recovery and isolation of H2S to be further converted to
various value-added products downstream, such as sulfur, hydrogen,
and other sulfur-containing composites/materials for circular economy
applications.
Credit author statement
Yi Herng Chan: Conceptualization, Writing – Original draft, Writing
– Review & Editing, Visualization Serene Sow Mun Lock: Writing –
Original draft, Writing – Review & Editing, Visualization Mee Kee
Wong: Writing – Original draft, Writing – Review & Editing, Visuali­
zation Chung Loong Yiin: Writing – Original draft, Writing – Review &
Editing, Visualization Adrian Chun Minh Loy: Writing – Original draft,
Writing – Review & Editing, Visualization Kin Wai Cheah: Writing –
Original draft, Writing – Review & Editing, Visualization Slyvester Yew
Wang Chai: Writing – Original draft, Writing – Review & Editing,
Visualization Claudia Li: Writing – Original draft, Writing – Review &
Editing, Visualization Bing Shen How: Writing – Original draft, Writing
– Review & Editing, Visualization Bridgid Lai Fui Chin: Writing –
Original draft Zhe Phak Chan: Writing – Original draft Su Shiung Lam:
Conceptualization, Writing – Review & Editing, Supervision.
Declaration of competing interest
The authors declare that they have no known competing financial
interests or personal relationships that could have appeared to influence
the work reported in this paper.
Data availability
No data was used for the research described in the article.
Acknowledgement
The authors gratefully acknowledge the support from the head of all
organizations involved and the permission to publish the findings. The
authors would like to thank The Education University of Hong Kong and
Universiti Malaysia Terengganu for the financial support under Inter­
national Grant (UMT/CRIM/2-2/25/JLD 8, Vot 53376). The work is also
supported by Program for Innovative Research Team (in Science and
Technology) in University of Henan Province (No. 21IRTSTHN020) and
Central Plain Scholar Funding Project of Henan Province (No.
212101510005).
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