120 (2023) 205152

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Gas Science and Engineering

journal homepage: www.journals.elsevier.com/gas-science-and-engineering

Recent progress and prospects in solid acid-catalyzed CO2 desorption from

amine-rich liquid
Shanlong An a, b, 1, Teng Xu a, b, 1, Lei Xing c, Guangfei Yu a, Rongzhe Zhang a, b, Jingwen Liu a, b,
Aizimaitijiang Aierken a, Qin Dai a, *, Lidong Wang a, b
a
MOE Key Laboratory of Resources and Environmental Systems Optimization, College of Environmental Science and Engineering, North China Electric Power University,
Beijing, 102206, China
b
Hebei Key Lab of Power Plant Flue Gas Multi-Pollutants Control, Department of Environmental Science and Engineering, North China Electric Power University,
Baoding, 071003, China
c
State Key Joint Laboratory of Environment Simulation and Pollution Control, School of Environment, Tsinghua University, Beijing 100084, China

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

Keywords: CO2 emissions from industrial processes and their impact on climate change have gradually become major
CO2 capture concerns. The amine-based scrubbing technology is considered a viable strategy for capturing CO2 to alleviate
Solid acid catalysts the climate crisis. However, the high expense of CO2 capture operations is severely hindering the further
CO2 desorption
development of this technology and its application in industry. The catalytic CO2 desorption strategy has recently
Amine regeneration
Energy consumption
attracted considerable attention recently as a low-energy technology, and it has high potential for large-scale
implementation. Therefore, in this review, we summarize the latest progresses in solid acid-catalyzed desorp­
tion of CO2 from various amine-rich liquids, especially monoethanolamine (MEA) solution. Solid acid catalysts
(SACs) are of six types: metal oxides, molecular sieves, natural clay minerals, composite materials, organic
framework materials, and carbon-based materials. These catalysts improve CO2 desorption through mechanisms
that are driven by Lewis acids, Brønsted acids, and basic active sites, as is discussed in depth in this paper. The
stability of the catalysts and their advantages and disadvantages are also considered. Finally, based on the
characteristics of various catalysts, we comprehensively compare and analyze their industrial potential and
provide some prospects regarding their future development. Moreover, to solve certain bottleneck problems in
this field, the application prospects of machine learning algorithms in CO2 desorption have been discussed.
Overall, this paper provides a robust theoretical basis and technical reference regarding efficient and inexpensive
carbon capture.

1. Introduction phased reduction of emissions (Bond and Sun, 2005; Wang et al.,
2023a). Finally, the global goal of carbon neutrality has been estab­
Global CO2 emissions related to energy increased from 24.3 Gt in lished. Given the background of a deteriorating global climate, a
2000 to 36.3 Gt in 2021, denoting an increase of approximately 50% consensus has been reached globally that CO2 emissions should be
(IEA, 2022). These emissions have resulted in the atmospheric CO2 reduced to address the climate crisis (Mathew, 2022; Ortega-Ruiz et al.,
concentration rising to 416 ppm and the average temperature increasing 2022).
by 1.01 ◦ C (Bajpai et al., 2022). The increase in CO2 emissions has 82.3% of energy that is consumed globally is obtained from fossil
triggered a series of ecological and environmental problems that are fuels (Gurney et al., 2009; Liu et al., 2019d). Given the current tech­
severely threatening human health and the development of society nological level of new sources of energy and related resource conditions,
(Chen et al., 2020a, 2022a). In response to global warming and the these new sources have not yet been developed on large industrial scales
greenhouse effect as well as through various climate conferences, and do not yet pose a major threat to traditional energy sources such as
countries worldwide have developed principles and targets aimed at the coal and petroleum. Thus, the carbon capture and storage (CCS)

* Corresponding author.
E-mail address: [email protected] (Q. Dai).
1
These authors contributed equally to this work.

https://doi.org/10.1016/j.jgsce.2023.205152
Received 13 May 2023; Received in revised form 5 October 2023; Accepted 17 October 2023
Available online 21 October 2023
2949-9089/© 2023 Elsevier B.V. All rights reserved.
S. An et al. Gas Science and Engineering 120 (2023) 205152

technology is a crucial strategy for controlling CO2 emissions and can be compression through drying and dehydrating, it can be subsequently
applied alongside clean energy (Dods et al., 2021; Zhang et al., 2022b). used or stored. The regenerated CO2-lean liquid is cooled by the lean­
The leading CCS technologies currently used for the capture of CO2 –rich liquid heat exchanger and then re-sent to the absorption tower for
emissions from industrial processes include precombustion capture, oxy- its reuse (Vaz et al., 2022).
fuel combustion capture, and post-combustion capture (Fig. 1a) (Helei First-generation amine absorbents are mainly single-component
et al., 2021). Of these, post-combustion capture is the most widespread amine absorbents—primary, secondary, or tertiary amines depending
because the technology can be retrofitted on the original equipment. on the number of active hydrogen atoms attached to the nitrogen (Aghel
Absorption is the most common mechanism underlying post-combustion et al., 2022). The absorbents most commonly used in industry are
capture (57% of post-combustion capture technologies), followed by monoethanolamine (MEA, a primary amine), diethanolamine (DEA, a
adsorption (14%), use of membranes (8%), and other mechanisms (21%; secondary amine), and methyldiethanolamine (MDEA, a tertiary
Fig. 1b) (Chao et al., 2021; Wilberforce et al., 2019). Chemical absorp­ amine). The reaction of a primary or secondary amine with CO2 first
tion in which amine is the absorbent has been discovered to be the most produces zwitterion intermediates (Wang et al., 2017); deprotonation of
feasible post-combustion capture technology owing to its fast absorption zwitterions then produces protonated amines and carbamates [Eqs. (1)
rate, excellent absorption capacity, and high adaptability to flue gas and (2)]. The theoretical CO2 absorption load for these reactions is 0.5
(Gao et al., 2020c). Absorption and desorption are typical processes in mol CO2/mol amine. In CO2 absorption, tertiary amines do not directly
the chemical absorption technology for CO2 capture (Gautam and react with CO2 to form zwitterions but instead serve as an alkaline
Mondal, 2023). After flue gas has undergone denitrification, dust catalyst that promotes the hydration of CO2 [Eq. (4)]; in this reaction,
removal, and desulphurization, it enters a regulating tower where it is the theoretical CO2 absorption load can reach 1.0 mol CO2/mol amine
cooled and the impurities are removed. Subsequently, the flue gas enters (Gautam and Mondal, 2023). In addition, 2-amino-2-methyl-1 propanol
the bottom of the CO2 absorption tower and flows upward; the absorbent (AMP), a sterically hindered amine, has received widespread attention
is sprayed at the top of the tower and reacts with the flue gas in reverse (Nwaoha et al., 2016). Its initial reaction with CO2 follows the zwit­
contact. Purified flue gas is discharged from the top of the absorption terionic absorption mechanism; in contrast to primary and secondary
tower. CO2-rich liquid flows to the bottom of the absorption tower and is amines, the nitrogen atom on the sterically hindered amine exerts a
then pumped through a lean–rich liquid heat exchanger into the strong steric hindrance effect; thus, the generated carbamate is
desorption tower, where it is heated by steam, causing release of CO2. extremely unstable and prone to hydrolysis, leading to the generation of
The desorbed CO2 is discharged from the top of the tower, and after its bicarbonate and a free amine. Therefore, in this reaction, the theoretical

Fig. 1. (a) Different systems of CCS; (b) post-combustion carbon capture technologies.

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S. An et al. Gas Science and Engineering 120 (2023) 205152

CO2 absorption load of a sterically hindered amine can reach 1.0 mol the CO2 from the amine-rich solution should be desorbed. The desorp­
CO2/mol amine. However, the use of a one-component amine for CO2 tion reaction contrasts to that of absorption Eqs. (5)–(7) (Chen et al.,
absorption has certain limitations; the chemical reaction rate of a pri­ 2022b). As indicated in Eqs. (5)–(7), the key step in CO2 desorption is
mary or secondary amine with CO2 is high, but the CO2 absorption load the disruption of the C–N bond in AmineCOO− and the prompt transfer
is low, the carbamate generated is stable in nature, and the temperature of the protons in AmineH+ 2 . CO2 desorption involves highly endothermic
required for desorption is high, resulting in high energy consumption reactions, and amines have limited ability to cause the transfer of pro­
(Ma et al., 2020). Tertiary amines and sterically hindered amines exhibit tons in AmineH+ 2 in alkaline solutions because amines are stronger
a higher CO2 absorption load and provide higher regeneration perfor­ Brønsted alkalis than is water. Additionally, HCO−3 can serve as a proton
mance for reaction products, but they are associated with the limitation acceptor, resulting in the lower activation energy of the deprotonation
of a low CO2 absorption reaction rate (Monteiro et al., 2013). reaction (Liu et al., 2017). Nevertheless, these absorbents contain few
To overcome the aforementioned limitation for single-component HCO−3 groups in the CO2-rich phase (Shi et al., 2014).
amines, researchers have proposed the second generation of amine ab­
AmineCOO− + H3 O+ ↔ AmineH + CO2 + H2 O (5)
sorbents. Mixed-amine absorbents typically combine a primary or sec­
ondary amine with a tertiary or sterically hindered amine to achieve a
AmineH+
2 + H2 O ↔ AmineH + H3 O
+
(6)
high CO2 absorption rate, a high CO2 absorption load, and excellent
regeneration performance (Mohd Rozaiddin and Lau, 2022; Shi et al.,
AmineH+ −
2 + HCO3 ↔ AmineH + CO2 + H2 O (7)
2014). However, mixed-amine absorbents generally have a high water
content; their potential for energy consumption reduction through To break the C–N bond and cause the transfer of the proton in
absorbent desorption is limited due to the large specific heat capacity of AmineH+ 2 , high temperature (110–130 C) is usually required in the
◦

water and the absorbents’ low boiling point. As a representative type of traditional noncatalytic desorption process (Wang et al., 2018). Such a
third-generation CO2-capture absorbents, biphasic absorbents have high temperature leads to the vaporization of water and amine, which
significant energy-saving potential and have received widespread leads to the consumption of some energy. With the most mature MEA
attention in recent years (Zhang et al., 2019a). Before CO2 absorption, a absorption technology, the energy consumed in the desorption processes
biphasic absorbent is a miscible solution, and after absorption of a can reach 3.6–4.0 GJ/t CO2 (Fig. 2), and this inevitably increases the
certain amount of CO2, liquid–liquid phase separation occurs. One of the operating cost by approximately 80% (de Meyer and Bignaud, 2022).
phases is enriched with CO2 (i.e., more than 90% CO2). Therefore, only Hence, the high energy demand has limited the development of
the CO2-rich phase must be sent to the desorption tower for regenera­ amine-based scrubbing technology (Borhani et al., 2018; Razi et al.,
tion; the CO2-lean phase can be directly returned to the absorption tower 2013). To solve this problem, various techniques for the regeneration of
for reuse, greatly reducing the desorption volume of the absorbent so­ amine solvents have been investigated. Table 2 provides a summary of
lution and thus effectively reducing the energy needed for regenerating the process characteristics and limitations of energy-efficient CO2
the absorbent (Wang et al., 2019). However, biphasic absorbents are desorption technologies.
generally associated with some problems, such as difficulty regulating Of the various technologies listed in Table 2, catalytic desorption by
the phase separation process and poor operational stability, and these a solid acid catalyst (SAC) has shown great potential. The addition of
problems limit their ability to reduce energy consumption (Liu et al., SACs accelerates the proton transfer process and the breakage of the N–C
2019a). Typical representatives of these absorbents are presented in bond in carbamate due to modulation of acidic sites on the catalyst
Table 1. surface (Alivand et al., 2020). Faster desorption of CO2 enables the faster
completion of the regeneration process, which reduces the time needed
AmineH + CO2 ↔ AmineH+ COO− (1)
to regenerate amines and the cycle time of the system, thus reducing
energy consumption for regeneration. A shorter regeneration residence
AmineH + AmineH+ COO− ↔ AmineCOO− + AmineH+ (2)
2
time leads to a smaller plate in the desorption tower, decreasing the
temperature at the bottom of the column and reducing the cost of the
AmineCOO− + H2 O ↔ AmineH + HCO−3 (3)
system. In addition, given the favorable characteristics of SAC, namely
the high activity, reusability, low environmental impact, and flexible
AmineT + H2 O + CO2 ↔ AmineT H+ + HCO−3 (4)
coupling with different amines, catalytic desorption is extremely
where AmineH, AmineT, and AmineTH denote a free amine, a tertiary promising for applications in industry. However, up-to-date systematic
amine, and the protonated tertiary amine, respectively (Meng et al., and comprehensive reviews of solid-acid-catalyzed CO2 desorption are
2022). lacking, particularly those covering novel materials (organic frame­
To recycle an absorbent and further utilize the CO2 absorbed on it, works, etc.) that have been reported from 2020 onwards. Therefore, this
paper summarizes the recent progress in SACs for the catalyzed

Table 1
Absorbents commonly used for CO2 capture in the chemical absorption method.
Type Composition Composition ratio CO2 load Reaction product Regeneration heat Ref.

Single amine MEA-H2O 30%–70% 0.52 mol/mol Carbamate, Protonated amine, HCO−3 /CO2-
3 3.60–3.80 GJ/t Kim et al. (2015)
DEA-H2O 34%–66% 0.53 mol/mol 3.4–3.7 GJ/t Galindo et al. (2012)
MDEA-H2O 30%–70% 0.52 mol/mol Protonated amine, HCO−3 /CO2-
3 1.19–1.34a GJ/t Chowdhury et al. (2011)
AMP-H2O 30%–70% 0.80 mol/mol 1.84a GJ/t El Hadri et al. (2017)
Mixed amine DETA-AMP-H2O 1 M–2M 2.49 mol/L Carbamate, Protonated amine, HCO−3 /CO2-
3 729.5 kJ/mol Wai et al. (2018)
MEA-AMP-PZ 3M-2.5M–0.5 M 0.57 mol/mol 287.1 kJ/mol Nwaoha et al. (2016)
DETA-PZ-H2O 20%-10%–70% 0.48 g/g amine 3.98 GJ/t Liu et al. (2019c)
Biphasic solvent AEEA-DEEA-H2O 20%-60%–20% 0.8–2.7 mol/kg Carbamate, Protonated amine, HCO−3 /CO2-
3 2.24 GJ/t Liu et al. (2019b)
MAPA-DEEA-H2O 2 M–5M ~5.00 mol/kg 2.20–2.40 GJ/t Pinto et al. (2014)
MEA-Sulfoalne-H2O 4 M–5M 3.88 mol/L 2.67 GJ/t Wang et al. (2018)
AEP-1-Propanol- 20%-40%–40% 1.26 mol/mol 2.74 GJ/t Shen et al. (2021)
H2O

MEA: monoethanolamine; DEA: diethanolamine; MDEA: N-methyldiethanolamine; AMP: 2-amino-2-methyl-1-propanol; DETA: diethylenetriamine; PZ: piperazine;
AEEA: 2-[(2-aminoethyl) amino] ethanol; DEEA: 2-(diethylamino)ethanol; MAPA: 3-(methylamino)-propylamine; AEP: N-aminoethylpiperazine. a: Absorption heat.

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S. An et al. Gas Science and Engineering 120 (2023) 205152

Fig. 2. Energy consumption of MEA regeneration.

desorption of CO2 from various amine-rich liquids. This review mainly 3. Six categories of SACs and modified composite materials
focuses on the following aspects: (1) a possible reaction mechanism of
catalytic CO2 desorption by SACs is proposed; (2) the catalytic perfor­ SACs can be divided into the following six categories based on their
mance and stability of six types of SAC at low desorption temperature structural characteristics: metal oxides, molecular sieves, natural clay
(<100 ◦ C) are demonstrated, the reason for the improvement in per­ minerals, composite materials, organic framework materials, and
formance relative to the noncatalytic condition is clarified, and the ad­ carbon-based materials (Liu et al., 2020; Sirsam et al., 2016). In the early
vantages and disadvantages of catalytic CO2 desorption are analyzed; stage of the related research, scholars mainly focused on single metal
and (3) on the basis of the comparative analysis of various desorption oxide and molecular sieve materials, but the activity and stability of
materials, the prospects for the future development of catalytic CO2 these catalysts have certain shortcomings. Therefore, a series of surface
desorption are proposed. This review aims to guide the design and modifications—such as loading, shell coating, and heterojunction
development of catalysts for their application to catalytic CO2 desorp­ engineering—have been adopted to improve catalytic performance and
tion in industry and to reveal the underlying mechanism in depth. promote CO2 desorption (Fu et al., 2021; Sun et al., 2022). The detailed
development of the six types of SAC is discussed in this section.
2. SAC-assisted catalytic desorption mechanism
3.1. Metal oxides and modified materials
An SAC is defined as a catalyst with abundant Brønsted acids (BASs,
including –OH, –SO3H, and -PO4H) or Lewis acids (LASs) (Nakajima and Metal oxides are widely used in various industrial applications as
Hara, 2012), which are mainly provided by unsaturated metal compo­ common SACs due to their easy synthesis and relatively low cost (Ali
nents (including ZrO2, TiO2, Al2O3, Fe3O4, MoO3, and CeO2; (Gupta and et al., 2022; Vasić et al., 2020). The unsaturated metal components on
Paul, 2014). The mechanism underlying SAC-catalyzed CO2 desorption the surface of metal oxides serve as electron acceptors to accelerate the
is illustrated in Fig. 3. BASs serve as proton donors (HB) on the catalyst disruption of the C–N bond in AmineCOO− , thus promoting CO2
surface and directly supply abundant free protons (H+) to convert desorption. Idem et al. (2011) discovered that γ-Al2O3 can effectively
AmineCOO− into AmineCOOH (Bhatti et al., 2023). The active sites of catalyze CO2 desorption, reducing the regeneration temperature of 5 M
the catalysts that donate protons (B− ) obtain acidic protons from MEA and decreasing the regeneration energy requirement by 27%. This
AmineH+ 2 [Eq. (8) and (9)] (Hou et al., 2022). discovery has made γ-Al2O3 a benchmark for further research. Wang
AmineCOO− + HB ↔ AmineCOO− H+ + B− (8) et al. (2016) used TiO2 and SiO2 to catalyze CO2 desorption. Compared
with γ-Al2O3, TiO2 and SiO2 were discovered to exhibit higher catalytic
B− + AmineH2 + ↔ AmineH + HB (9) performance (TiO2 > SiO2 > γ-Al2O3. The introduction of TiO2 short­
ened the regeneration time by up to 42%. However, according to Wang
LASs serve as proton acceptors (L− ) of protons from AmineH+2 ; these et al. (2016), the improved performance was solely due to the increase in
protons are then donated to water, thereby accelerating the desorption the mass transfer efficiency by TiO2 nanoparticles; the catalytic action of
process [Eq. (10) and (11)] (Gecim et al., 2022). the catalysts was neglected in that study. Transition metals with d-or­
AmineH2 + + L− ↔ HL + AmineH (10) bitals or empty orbital can easily provide and accept electrons, making
them appropriate desorption catalysts. For example, in 2017, Bhatti and
HL + H2 O ↔ L− + H3 O+ (11) colleagues studied the effect of transition metal oxides such as MoO3,
V2O5, Cr2O3, Ag2O, ZrO2, and CuO on MEA regeneration. They
Moreover, the oxygen atom of AmineCOO can be chemisorbed onto
−
demonstrated that MoO3, Ag2O, and ZrO2 exhibited excellent catalytic
the metal components (LASs) of the catalysts. Subsequently, protons are activity, leading to 100%–200% enhancement of the CO2 desorption
transferred from the oxygen atom to the nitrogen atom through the rate compared with noncatalytic conditions and reducing the MEA
isomerization process, leading to destruction of the delocalized conju­ regeneration temperature to less than 100 ◦ C, thus effectively reducing
gation of nitrogen atoms. Subsequently, the C–N bond is disrupted the energy consumed in desorption (Table 3) (Bhatti et al., 2017, 2018a,
(Srisang et al., 2018). 2018b). The higher catalytic desorption performance of MoO3 and V2O5
than that of single LAS catalysts (Cr2O3, TiO2, WO3, etc.; MoO3 > V2O5
> Cr2O3 > TiO2 > WO3 > no catalyst) is attributed to the presence of

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S. An et al. Gas Science and Engineering 120 (2023) 205152

Table 2 showed that the CO2 desorption rate could be increased by 4500% and
Process characteristics and limitations of energy-efficient CO2 desorption the desorption amount increased by 75%, considerably reducing energy
technologies. consumption and amine losses. This was because the –OH group in TiO
Desorption Process Difficulties and Ref. (OH)2 donated and received protons, accelerating the reactions
technology characteristics limitations involving protons (i.e., protonation and deprotonation). Moreover, the
Traditional Desorbing CO2 High desorption Gecim et al. (2022) excellent stability of the catalyst was confirmed through 50 cyclic CO2
thermal through temperature, absorption–desorption experiments. Viscardi et al. (2020) enriched
desorption traditional volatile absorbent, catalysts with BASs through the introduction of sulfonic acid groups
heating. and high overall
(-SO3H), which enhanced their catalytic performance. Li et al. (2018)
energy
consumption. prepared SO2−4 /TiO2 for catalytic CO2 desorption by calcining industrial
Desorption CO2 is absorbed The new amine (Guo et al., 2019; rough metatitanic acid at 400–600 ◦ C. The CO2 desorption rate driven
from new using new amine solvents are costly Wang et al., 2021b; by SO2−4 /TiO2 was 28.9% higher than that under noncatalytic condi­
amine solvents such as and prone to Zhou et al., 2021) tions. After four cycles, the performance decreased by more than 4%.
solvents MDEA, DETA, degradation and
nonaqueous corrosion. Non-
Zhang et al. (2017) synthesized SO2− 4 /ZrO2 through the reaction of
solvents, for aqueous solvents amorphous ZrO2 with sulfur compounds at high temperature. The
which desorption are toxic and addition of SO2−4 /ZrO2 resulted in 14.1% greater CO2 desorption and
can be performed flammable. 17.1% lower regeneration heat duty compared with noncatalytic con­
at lower
ditions. Despite the advantages of SO2−4 /MxOy, these catalysts have the
temperature and
the energy problem of easy loss of active sites after multiple cycles because the
consumed in sulfated materials are sensitive to water (Li et al., 2019; Xu et al.,
regeneration can 2018a).
be reduced. The participation of metal oxides and their modifications in the CO2
Catalytic A catalyst is added The main difficulty Mohd Rozaiddin and
desorption reaction can promote CO2 desorption to a certain extent.
desorption to boost the CO2 lies in exploiting Lau (2022)
desorption catalysts with However, the specific surface area of these materials is small (<100 m2/
reaction and lower excellent catalytic g), and they have nonuniform pore size distributions. Their active sites
the regeneration performance and mainly consist of single and limited LASs, and they are deactivated
energy demand. stability.
under high-temperature and alkaline conditions. Qualitative and quan­
Membrane During CO2 Although they (Koonaphapdeelert
desorption desorption, reduce energy and Li, 2006; Xu titative analyses of SAC phosphorylation sites are yet to be conducted.
gas–liquid consumption, most et al., 2018b; Zhao For instance, temperature-programmed desorption of ammonia (NH3-
membrane polymer et al., 2016) TPD) analysis can be employed to measure both the density and strength
contactors can be membranes are of the acid sites in SACs (Niwa and Katada, 2013), whereas pyridine
employed for unstable at
infrared (Py-IR) can be utilized to differentiate between the BASs and
direct CO2 relatively high
stripping (i.e., temperature. LASs present in SACs (Hughes et al., 1969). Furthermore, an overall
regenerating the Moreover, mass understanding of the catalytic desorption mechanism at the molecular
liquid absorbent) transfer efficiency level and of the structure–activity relationship is necessary if more
and simultaneous is low due to pore
efficient and sustainable SACs are to be developed. Metal oxides can
heat recovery. The contamination and
CO2 transfer membrane wetting.
catalyze the regeneration of mixed amines, but their efficacy is inferior
occurs in the to that of molecular sieve catalysts, which are discussed next.
opposite direction
from the liquid to 3.2. Molecular sieves and modified materials
the gas phase and
is driven by the
difference in CO2 Molecular sieves are crystalline aluminosilicate materials, mainly
partial pressure composed of silicon, aluminum, and oxygen atoms (Chen et al., 2020b;
across the Wang et al., 2021a). They are characterized by uniform pore size, high
membrane.
stability, and favorable crystallinity (Gao et al., 2023; Ma et al., 2023).
Moreover, metal atoms (e.g., Al) and –OH groups in molecular sieves can
both LASs (M–O, M = Mo, and V) and BASs (-OH in M–OH, M = Mo, and act as LASs and BASs, respectively (Chen et al., 2017; Lu et al., 2022).
V). BASs may be more favorable for CO2 desorption at low temperature These properties make molecular sieves excellent catalysts and carriers.
because BASs have high acid strength and activity, providing an HZSM-5 exhibits high selectivity, a favorable silicon-to-aluminum ratio,
adequate number of acid sites. Furthermore, the performance of metal and adjustable acidity; thus, it is the most prevalent molecular sieve
oxide catalyst regeneration is influenced by the coordination number catalyst employed for CO2 desorption. Its CO2 desorption catalytic
and geometry of the metal. For instance, NiO and MnO2 exhibit octa­ performance has been reported to surpass that of γ-Al2O3 (Li et al.,
hedral coordination with six oxygen atoms, whereas Nb2O5 and CuO 2022a; Srisang et al., 2017). Osei et al. (2017) confirmed that in 5 M
exhibit square planar coordination with four oxygen atoms coordinated MEA solution, HZSM-5 exhibited higher catalytic activity than γ-Al2O3
with metal atoms. Ag2O exhibits linear geometry with two-coordinate owing to its superior mass transfer coefficient and more numerous BASs.
Ag centers connected by tetrahedral oxides. Their reactivity after their To further improve the catalytic characteristics of HZSM-5, alkaline
regeneration from the MEA solvent follows the order: Ag2O > Nb2O5 > desilication can be performed to enhance its mesoporosity and surface
CuO > NiO > MnO2. Ag metal atoms can coordinate with four carba­ acidity. Bhatti et al. (2020b) synthesized a range of mesoporous HZSM-5
mate groups and withdraw electrons from nitrogen atoms, significantly materials (HZ-x, where x indicates the alkali concentration) through an
enhancing CO2 desorption (Bhatti et al., 2018b). easy alkaline desilication and surfactant-induced reassembly technique.
Given the important but limited active acid sites on metal oxides, The resulting catalysts had higher mesoporosity and more abundant
researchers have enriched catalysts with BASs by introducing extra BASs than HZSM. Experimental results revealed that for catalytic
surface groups (e.g., –OH, –SO3H, SO2−4 ) through modification (Dhar­
desorption at <82 ◦ C, HZ-x led to 60% more CO2 desorption and 24%–
malingam et al., 2022). For example, Lai et al. (2018) investigated 37% lower heat duty relative to noncatalytic conditions (Table 4). The
nano-TiO(OH)2 for catalytic CO2 desorption. The experimental results catalysts offered protons and Al atoms for attacking the nitrogen atom in
carbamate and thus cause the breakage of the N–C bond. SAPO-34 and

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S. An et al. Gas Science and Engineering 120 (2023) 205152

Fig. 3. Mechanism of CO2 desorption catalyzed by LASs and BASs of SACs.

Table 3
Catalytic desorption performance of metal oxides.
Catalysts Desorption temperature (◦ C) Des. Rate increment Des. Amount increment Heat duty reduction Ref.

Non-catalyst – 0% 0% 0% –
TiO(OH)2 88 4500% 75% – Lai et al. (2018)
MoO3 86 45% 50–83% saved 48% of sensible heat Bhatti et al. (2017)
V2O5 86 28% 50–95% saved 44% of sensible heat Bhatti et al. (2017)
Ag2O 80 218% 48% – Bhatti et al. (2018b)
Nb2O5 80 – 46% – Bhatti et al. (2018b)
CuO 80 – 23% – Bhatti et al. (2018b)
MnO2 80 – 30% – Bhatti et al. (2018b)
ZrO2 86 54% 31–32% – Bhatti et al. (2018a)

Table 4
Catalytic desorption performance of molecular sieve materials.
Catalysts Absorbent Desorption temperature Des. Rate Des. Amount Relative heat Acid site B/L (mmol/ Ref.
(◦ C) increment increment duty g)

Non-catalyst – – 0% 0% 100% – –
HZSM-5 MEA 82 33.0% 30.9% 70.8% 0.198/0.268 Bhatti et al.
(2020b)
HZ-0.2 MEA 82 – 24% 76.2% 0.293/0.099 Bhatti et al.
(2020b)
HZ-0.5 MEA 82 83.4% 59.2% 62.7% 0.428/0.163 Bhatti et al.
(2020b)
HZ-0.7 MEA 82 97.9% 54.3% 67.2% 0.430/0.118 Bhatti et al.
(2020b)
SAPO-34 MEA 96 28.3% 28.3% 75.7% 1.082/0.741 Zhang et al.
(2017)
SBA-15 MEA 97.5 – 14.8% 81% 0.49/0.09 Gao et al. (2020b)
MCM-41 MEA 90 – 13.15% 89.2% – Sun et al. (2021)
SAPO-34 DEAPA 90 71.2% 71.8% 66.92% 1.46 Hu et al. (2019)
MCM-41- MEA 90 195% 52.6% 66.7% – Sun et al. (2021)
SO3H
HZSM-5 MEA/MDEA 98 107.4% 107% 48.8% – Liu et al. (2017)
HZSM-5 MEA/AMP/PZ 96 121.2% 173.2% 61.6% 1.51 Zhang et al.
(2018b)
Hβ MEA/MDEA/ 98 100.3% 147.3% 66.1% – Zhang et al.
PZ (2019b)
HND-8 MEA/BEA/ 90 – – 53.4% – Shi et al. (2022)
DEEA
HND-8 MEA/EAE/ 90 – – 63.8% – Zhang et al.
AMP (2022a)

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S. An et al. Gas Science and Engineering 120 (2023) 205152

SBA-15 have also been extensively employed for CO2 catalytic desorp­ was 48.8% lower for this system than for noncatalytic MEA. The high
tion. Zhang et al. (2017) reported that the introduction of SAPO-34 led CO2 desorption performance was attributed to the strong
to 28.3% higher CO2 desorption efficiency and 24.3% lower thermal electron-absorbing chemical structure of MDEA. Regarding trisolvent
load compared with those for no catalysis. Hu et al. (2019) demon­ absorption systems, Zhang et al. (2018c) examined energy consumption
strated that the utilization of SAPO-34 also led to less energy con­ for the regeneration of mixed-amine system comprising 3 M MEA, 2.5 M
sumption for CO2 desorption from amines other than MEA 2-amino-2-methyl-1-propanol (AMP), and 0.5 M piperazine (PZ) that
[3-(diethylamino)propylamine (DEAPA)], except for MEA solution. Gao was catalyzed by HZSM-5, and the results revealed that the relative heat
et al. (2020b) employed SBA-15 to catalyze MEA regeneration and found duty was 61.6% lower for this system than under noncatalytic MEA
that it reduced heat duty by 19%. conditions. Zhang et al. (2019a) also examined the effect of a molecular
Surface (-SO3H) modification has been demonstrated to be a highly sieve catalyst containing 3 M MEA, 2.5 M MDEA, and 0.5 M PZ on CO2
promising approach to further enhancing the acidity of molecular sieve desorption performance. Of the catalysts tested, the H-Beta (Hβ) catalyst
materials. For example, Sun et al. (2021) prepared combined with mixed amines exhibited the highest regeneration per­
sulfonic-acid-functionalized MCM-41 (MCM-41-SO3H) and found that it formance. Compared with those in the MEA blank run, the CO2
exhibited high catalytic activity for CO2 desorption. The CO2 desorption desorption performance was 1360.8% higher, and relative regeneration
capacity of MCM-41-SO3H was four times higher than that of the un­ energy was 66.1% lower. The ratios of different amines in various
modified catalyst, and the relative heat load was more than three times mixed-amine systems, along with their effective integration with
smaller. Theoretical calculations revealed that the ΔH value (where ΔH different molecular sieve catalysts, are key factors for optimizing cata­
represents the reaction enthalpy of CO2 desorption) of MCM-41-SO3H lytic performance. In CO2 desorption experiments, Shi et al. (2022) used
(− 0.39 eV) was considerably lower than that of MCM-41 (1.15 eV). This a three-phase solvent—comprising MEA, butylethanolamine (BEA), and
observation suggests that MEACOO− is more likely to decompose ther­ MDEA—in combination with five commercial catalysts:
modynamically on the MCM-41-SO3H catalyst than on MCM-41. The γ-Al2O3/HZSM-5, H-beta, H-mordenite, HND-8, and HND-580. The
calculated Bader electron number for the acidic H site on the catalyst optimal combination was the trisolvent combined with HND-8, which
before and after the regeneration reaction revealed that the acid site H in resulted in 46.6% lower relative heat duty than that in the MEA blank
MCM-41-SO3H (0.21 protons) donated more protons than did MCM-41 run. Similarly, Zhang et al. (2022a) explored the catalytic effect of the
(0.17 protons; Fig. 4). The combined experimental results and theoret­ aforementioned five catalysts in a system comprising MEA, 2-(ethyl­
ical calculations indicated that the introduction of –SO3H enriched the amino) ethanol (EAE), and AMP and discovered that HND-8 exhibited
catalyst with BASs, increasing the total capacity of acid sites from 0.19 the highest catalytic effect, with the heat duty being reduced from 924.1
to 5.27 mmol/g, markedly decreasing the MEA regeneration energy, and to 589.3 kJ/mol.
effectively promoting CO2 desorption. However, after five cycles of ex­ In summary, molecular sieves and their modifications can facilitate
periments, catalytic performance decreased (the desorption amount CO2 desorption and can even outperform metal oxides. These molecular
decreased from 96 to 88 mmol), perhaps because of loss of S from the sieve catalysts also exhibit higher catalytic performance than metal
catalyst surface. Therefore, the stability of the sulfonic-acid-based oxides do in mixed-amine systems. By combining a mixed amine with
modified catalyst in alcohol–amine solutions will be improved in such a catalyst, energy consumption can be reduced to less than 50%.
future work. However, the following aspects must be addressed in future work: (1)
Molecular-sieve-catalyzed regeneration of amines in mixed-amine the loss of surface S must be slowed or prevented; (2) other stable acidic
systems exhibit reduced energy consumption. For example, Liu et al. sites (HCl, HNO3, H3PO4, etc.) should be incorporated to investigate the
(2017) reported that HZSM-5 demonstrated high performance in a impact of the modified acid type and quantity on catalytic activity; and
mixed-amine system comprising 5 M MEA + 1 M MDEA. The CO2 (3) sulfonated molecular sieve materials should be applied to mixed-
desorption rate was 107% higher and regeneration energy consumption amine systems.

Fig. 4. Structures of MEACOO− decomposition on (a) MCM-41 and (b) MCM-41-SO3H. Copyright ACS 2021; Sun et al., 2021).

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S. An et al. Gas Science and Engineering 120 (2023) 205152

3.3. Natural clay and modified materials (Table 5). After five cycles, the CO2 desorption amount decreased from
7.63 to 7.13 mmol, which suggests that active components will
Natural clay materials such as montmorillonite (Mont) and atta­ agglomerate after a certain number of cycles.
pulgite (ATP) exhibit molecular-sieve-like structures (Rashwan and Abd Natural clay materials are being used for an increasing number of
El-Shakour, 2022; Tao et al., 2022). Their large specific surface area, catalytic reactions due to their low cost and wide availability (Hambali
sizable micropores, low cost, environmentally friendliness, high thermal et al., 2022; Yaghmaeiyan et al., 2022). They also offer a route to the
stability, and metal ions that are exchangeable between layers make industrialization of energy-efficient carbon capture. However, the CO2
them potential catalysts for multiphase catalytic reactions (Lin et al., desorption ability of natural clay materials is constrained due to its
2016; Thao and Nhu, 2018). The –OH groups in the structure of natural limited number of total acid sites. Because of the presence of finite active
clay materials serve as BASs, and unsaturated metal ions exposed on the components (Si and Al) between the layers in natural clay, its activity is
surface serve as LASs, which collectively facilitate CO2 desorption relatively low. The activity of SACs can be improved by introducing
(Fig. 5) (Lu et al., 2021; Zhang et al., 2020a). The specific surface area stronger active metal components through ion exchange and other
and active acid sites of natural clay materials are essential for desorp­ methods.
tion. Tan et al. (2022b) examined the use of three clay materials for
catalytic CO2 desorption: ATP, activated bentonite (K-10), and sepiolite
3.4. Metal oxide-molecular sieve/natural clay composite materials
(SEP). The catalytic CO2 desorption performance followed the order
ATP > K10 > SEP. ATP exhibited the highest catalytic performance; it
Recent studies have focused on developing more efficient composite
increased the desorption rate by 54%–57% and reduced the relative heat
catalysts by combining the advantages of both metal oxides and mo­
duty by 32%. The amount of desorbed CO2 was slightly decreased (by
lecular sieves or natural clay materials through methods such as doping,
5%) after 15 cycles. Its highest performance was attributed to the large
recombination, and loading (Bao et al., 2017). Zhang et al. (2020b) used
surface area (88.9 m2/g) and highest number of moderate acid sites
three metals (Fe, Al, and Mo) to modify MCM-41. The performance of
(0.744 mmol/g). The study indicates that acid activation can enhance
the modified catalysts followed the order MCM41-Fe (M-Fe) >
the activity of natural clay materials by increasing their surface area and
MCM41-Al (M-Al) > MCM41-Mo (M-Mo) > MCM-41. At 98 ◦ C, the CO2
acidity. Bhatti et al. (2020a) employed HCl, HNO3, and H3PO4 for the
desorption rate and catalysis capacity of M-Fe were 52.5% and 49.3%
simple acid activation of Mont. Compared with Mont without any
higher and its relative heat duty was 32.5% lower than catalysis by
modification, the resulting catalysts had significantly higher BET surface
MCM-41. The excellent catalytic effectiveness of M-Fe was attributed to
area and mesoporosity, indicating the presence of more BASs and LASs.
its numerous BASs and Lewis basic sites. The basic groups participate in
The ranking of CO2 desorption performance was PO4-Mont > H-Mont >
the deprotonation reaction, in which they obtain acidic protons from
NO3-Mont. After H3PO4 activation, PO4-Mont exhibited the highest
MEAH+ and then transfer them to MEACOO− (Fig. 6a). However, only
catalytic desorption performance due to its large specific surface area
80% of the catalytic activity was retained after five cycles. The slight
(141.18 m2/g) and the most total acid sites (0.434 mmol/g) at 86 ◦ C
decline in catalytic activity may have been due to the collapse of the

Fig. 5. Mechanism of ATP catalytic desorption of CO2. Copyright Elsevier 2022; Tan et al., 2022b).

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S. An et al. Gas Science and Engineering 120 (2023) 205152

Table 5
Catalytic desorption properties of natural clay materials.
Catalysts Desorption temperature (◦ C) Des. Rate increment Des. Amount increment Relative heat duty Acid site B/L (mmol/g) Ref.

Non-catalyst – 0% 0% 100% – –
ATP 88 54–57% 48–50% 68% – Tan et al. (2022a)
K-10 88 – 38.5% 72.3% – Tan et al. (2022a)
SEP 88 – 18.1% 82.2% – Tan et al. (2022a)
Mont 86 13.4% – 88.1% 0.157/0.002 Bhatti et al. (2020a)
H-Mont 86 55.4% 29.6% 77.1% 0.257/0.086 Bhatti et al. (2020a)
NO3-Mont 86 47.7% 16.5% 85.9% 0.312/0.092 Bhatti et al. (2020a)
PO4-Mont 86 75.0% 47.9% 67.6% 0.329/0.105 Bhatti et al. (2020a)

Fig. 6. (a) A possible catalytic mechanism of CO2 desorption in MEA solution over M-Fe catalyst. Copyright Elsevier 2020; Zhang et al., 2020b). (b) Calculation
model of CO2 desorption for the SZ@H-x catalyst. Decomposition of RNHCOO− on different acid sites. Copyright ACS 2020; Xing et al. (2020b). (c) A plausible
reaction mechanism for MEACOO− breakdown facilitated by ion-exchanged Mont catalyst and the subsequent release of CO2 from CO2-rich MEA solution. Copyright
Elsevier 2021; Bhatti et al. (2021c).

catalyst structure to a certain degree. Huang et al. (2021) synthesized applied for CO2 desorption. At 96 ◦ C, Al-ZSM exhibited higher catalytic
β/SBA-15 (BS) Fe–Zr@BS through a hydrothermal method. Using activity then Al2O3 and HZSM-5; additionally, Al-ZSM saved approxi­
Fe–Zr@BS for CO2 desorption at 97 ◦ C resulted in a 112% increase in the mately 202.1 and 228.6 kJ/mol of CO2 heat duty relative to Al2O3 and
CO2 desorption factor and a reduction in the regeneration heat load to HZSM-5, respectively. The higher catalytic activity of Al-ZSM was
67%. However, when SBA-15 was used as the catalyst, the CO2 ascribed to the favorable synergistic effect between Al2O3 and HZSM-5,
desorption factor increased by only 19%, and the relative heat duty the greater mesopore surface area, and the greater number of BASs and
decreased to 87%. The increased catalytic capability was attributed to Lewis basic sites. SO2−
4 /ZrO2 has been extensively used as a component
the more numerous acid sites of Fe–Zr@BS than those of SBA-15. Zhang of composite materials because of its potent antioxidant properties and
et al. (2018b) utilized the precipitation ultrasonic method to synthesize abundant acidic sites (Li et al., 2023). Scholars have prepared solid
a set of Al2O3/HZSM-5 (Al-ZSM) bifunctional catalysts, which were super acid catalysts (H0 < − 11.9, where H0 is the Hammett acidity

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S. An et al. Gas Science and Engineering 120 (2023) 205152

function; (Knaeble and Iglesia, 2016) by loading SO2− 4 /ZrO2 onto CO2 (for the no-catalyst case) to 62 kJ/mol CO2, and the excellent cat­
HZSM-5 (Xing et al., 2020a), MCM-41 (Zhang et al., 2019c), SBA-15 alytic performance was attributed to abundant BASs and large pores in
(Gao et al., 2020b), SiO2 (Ali Saleh Bairq et al., 2019) and γ-Al2O3 the catalyst.
(Zhang et al., 2018a), . The composite modification greatly enriched the In summary, in composite catalysts, synergy between multiple active
catalyst surface with BASs and LASs, considerably improving the CO2 components provides more numerous acid sites and a larger specific
desorption efficiency and reducing the thermal load (Table 6). These surface area, thus improving the activity of SACs (Jing et al., 2019). The
experiments have also verified that SACs do not negatively affect the carrier enhances the scattering of active ingredients, which can inhibit
CO2 absorption process of MEA. Notably, Xing et al. (2020) found that agglomerative deactivation of metal oxides under high-temperature
unsaturated coordinated ions (Sin+ and Zrn+) in SO2− 4 /ZrO2-HZSM-5 alkaline conditions and thus prevent the catalyst from becoming un­
interact robustly with water molecules in the liquid phase, leading to the stable. The relatively low cost of composite catalysts renders it a
existence of groups (Si–OH and Zr–OH) that convert LASs into BASs in promising candidate for the industrial development of catalytic CO2
the desorption reaction (Fig. 6b). desorption.
In addition to composites combining molecular sieves with metal
oxides, composite materials combining natural clay with metal oxides
3.5. Organic frame materials and derivatives
also exhibit excellent catalytic activity. (Bhatti et al., 2021a, 2021b)
employed ion exchange to prepare a sequence of M-Mont catalysts (M =
The development of novel solid acid materials for catalytic CO2
Cr, Fe, Co, or Zr), which exhibited excellent catalytic desorption per­
desorption is a future research direction. Metal–organic framework
formance. The performance of each catalyst followed the order of
materials (MOFs) and covalent organic framework materials (COFs) are
Fe-Mont ≈ Zr-Mont > Co-Mont > Cr-Mont. Fe-Mont exhibited the
promising multifunctional precursors in the synthesis of nanomaterials
highest catalytic activity. According to experimental results, Fe-Mont
owing to their unique chemical structure, well-distributed porosity,
exhibited a CO2 desorption rate that was four times more than that of
large surface area, and flexible designability. Because the organic li­
Mont, and the catalysts exhibited favorable cycling stability. After five
gands present in MOFs and COFs are difficult to stabilize in high-
cycles, the catalyst activity decreased by only 4%–7%, and the charac­
temperature and highly alkaline environments, researchers have pre­
terization results indicated no noticeable changes to the catalyst struc­
pared SACs through modification or high-temperature calcination of
ture. Through ion exchange, most of the cations between parent Mont
organic framework materials (Guo et al., 2022; He et al., 2021; Wu et al.,
layers were replaced with active metal components, and the surface area
2020). To validate the feasibility of using MOF-derived catalysts for CO2
was simultaneously increased (24.4 m2/g for parent Mont, increasing to
desorption, Xing et al. (2021b) reported a “shell-covering” strategy for
34–223 m2/g) due to structural changes resulting from surface charge
constructing a robust MOF-derived nanocomposite named
properties during the ion exchange and the enhancement of the total
SO2−
4 /ZIF-67-C@TiO2 (SZC@TiO2). Under catalytic conditions at 88 C,
◦
number of acid sites, which significantly affects the CO2 desorption ef­
the catalyst provided a 153% increase in the CO2 desorption rate and a
ficiency (the catalytic mechanism is shown in Fig. 6c.). A study
64.5% increase in the desorption amount compared with noncatalytic
demonstrated that SnO2 has more strong acid sites than do ZrO2 and
conditions. Furthermore, the relative heat duty was reduced by 36%.
TiO2 (Heda et al., 2019). Tan et al. (2023) reported that the SnO2-mo­
After 10 cycles, the catalytic capacity of SZC@TiO2 was diminished by
dified ATP catalyst (SnO2/ATP) facilitated CO2 desorption at 88 ◦ C.
17%, demonstrating the high stability of this catalyst at the high tem­
Their experimental results showed that 1/2-SnO2/ATP led to a 265%
perature for regeneration. As illustrated in Fig. 7a and b, density func­
higher CO2 desorption rate and 101% greater amount of desorbed CO2 in
tional theory calculations proved that the participation of Co–Nx as an
contrast to the result for no catalyst; in addition, the energy requirement
electron acceptor in the catalytic process mediated the elongation of the
was reduced to 48.2%. The catalytic performance of 1/2-SnO2/ATP
N–C bond, resulting in a decomposition energy barrier of only 0.53 eV,
exceeded that of most catalysts in the literature, meaning that
which was considerably lower than that in the noncatalytic process
1/2-SnO2/ATP is one of the most promising candidates for industriali­
(0.91 eV). The lower reaction energy barrier implies higher desorption
zation. However, the results of cycle stability experiments for this
efficiency, which explains the excellent performance of the catalyst.
catalyst were not satisfactory. The catalytic performance of
Notably, similar desorption performance could be achieved with a much
1/2-SnO2/ATP decreased by approximately 20% after 12 cycles. None­
lower amount of this catalyst (0.01 wt%) compared with the amounts of
theless, the composite catalyst not only exhibited high catalytic per­
other catalysts (1.25–5 wt%). This would lead to the lower cost of the
formance in single-MEA systems but also considerably enhanced CO2
catalyst, promoting its practical application. Because of the excellent
desorption from mixed-amine systems. Prasongthum et al. (2019) syn­
catalytic performance of the core–shell MOF–derived catalysts, Alivand
thesized the solid super acid catalyst Ce(SO4)2/ZrO2 for use in the cat­
et al. (2022) synthesized a series of water-dispersible core–shell
alytic BEA-AMP system. The thermal load was reduced from 110 kJ/mol
MOF–derived nanocatalysts. They demonstrated that the functionalized

Table 6
Desorption performance of composites.
Catalyst Desorption Catalytic performance Recyclability Acid site B/L Ref.
temperature (◦ C) (mmol/g)

SO2−
4 /ZrO2-HZSM-5 98 The CO2 desorption rate and desorption capacity were increased 85% of catalytic activity 0.022/0.383 Xing et al.
(SZ@H-1/4) by 37% and 40%, respectively, and the relative heat duty was was retained after 5 cycles (2020a)
reduced by 31%.
SO2−
4 /ZrO2/MCM- 98 The CO2 desorption rate and desorption capacity were increased 92% of catalytic activity 3.854/1.898 Zhang et al.
41/Fe (SZMF10%) by 51.8% and 54.7%, respectively, and the relative heat duty was was retained after 4 cycles (2019c)
reduced by 28%–40%
SO2−
4 /ZrO2/SBA-15 97.5 The CO2 desorption factor was increased by 100%–200%, and the 95.9% of catalytic activity 2.32/4.15 Gao et al.
(SZS (2/1)) relative heat duty was reduced by 20%–26.5%. was retained after 4 cycles (2020b)
SO2−
4 /ZrO2/SiO2 97 The CO2 desorption rate and desorption capacity were increased 81% of catalytic activity 0.502/0.541 Ali Saleh Bairq
(SZS15%) by 35.1% and 66.7%, respectively, and the relative heat duty was was retained after 10 cycles et al. (2019)
reduced by 36.48%.
SO2−
4 /ZrO2/γ-Al2O3 98 The CO2 desorption rate and desorption capacity were increased 80% of catalytic activity 0.493/0.448 Zhang et al.
(SZA1/1) by 33.9% and 34.0%, respectively, and the relative heat duty was was retained after 4 cycles (2018a)
reduced by 24.9%–36.9%.

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S. An et al. Gas Science and Engineering 120 (2023) 205152

Fig. 7. (A) Relative energy and simplified surface structure of the various reaction species along the reaction pathway. Copyright ACS 2021; Xing et al. (2021b). (b)
CO2 desorption promoted by a robust MOF derivant. Copyright ACS 2021; Xing et al. (2021b). (c) Reactants and products for the decomposition of MEACOO− on a
Fe3O4@UiO-66-SO4 defect active site. Copyright Nature 2022; Alivand et al. (2022). (d) Catalytic mechanism diagram of CeM-HPW. Copyright Elsevier 2022; Wei
et al. (2022b). (e) SEM and TEM images and energy-dispersive X-ray spectroscopy elemental mapping of Co–C–N NSs. Copyright ACS 2022; Xing et al. (2022a). (f)
Calculation model of CO2 desorption for the NiFe2O4 catalyst; the model involves protonation of RNHCOO− and deprotonation of MEAH+. Copyright Elsevier 2022;
Li et al. (2022b).

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S. An et al. Gas Science and Engineering 120 (2023) 205152

nanoclusters (Fe3O4–COOH) were effective in mediating missing-linker they have a uniformly dispersed coordination structure containing
deficiencies and mesoporosity during the self-assembly of the MOF. The various metals, thereby enhancing the stability of catalytic sites (Gao
grown mesoporous shells facilitated the subsequent coordination of et al., 2020a). Li et al. (2022b) prepared coral-like SACs by covering
chelated sulfate groups on the metal clusters, leading to more numerous nanoscale NiFe2O4 clusters with COFs through a heterojunction engi­
BASs in and improved proton-donating ability of the catalyst (Fig. 7c). neering strategy. The relative heat duty was reduced to 42.45% under
Using only 0.1 wt% Fe3O4@UiO-66-SO4 at 88 ◦ C led to 44% lower catalytic conditions. As displayed in Fig. 7f, the coordination of M-N-(M)
relative heat duty than in the no-catalyst case, and the catalyst was (M = Ni or Fe) bonds in the NiFe2O4 cluster and COF supporter promotes
favorably recoverable (only 9% loss after five cycles). Multiple-scale the transformation of LASs into high-quality BASs. These abundant BASs
characterization revealed that the missing-linker defects and super­ facilitate efficient proton transfer, ensuring the rapid decomposition of
acidic sites throughout the hierarchical network of Fe3O4@UiO-66-SO4 MEACOO− and rapid CO2 desorption.
were critical factors determining its strong proton donation ability. In summary, the involvement of MOFs, COFs, and their derivatives
Heteropolyacid modification is an effective approach for enhancing the can significantly improve the CO2 desorption kinetics at a low dosage
acidity of catalysts. Catalysts modified in this way are outstanding cat­ (only 0.1 wt% compared with conventional catalysts, which are injected
alytic materials that offer benefits including high catalytic activity, high at more than 1.25 wt%) and exhibit excellent catalytic desorption per­
selectivity, and low corrosion and contamination. Wei et al. (2022a) formance (Table 7). The stability of these catalysts can be further
prepared the composite catalyst CeM–phosphotungstic acid (HPW) as a enhanced through modifications such as shell coating and hetero­
Ce-based MOF material to overcome the performance shortcomings of a junction engineering strategies (Murtaza et al., 2023). Organic frame­
single type of catalyst. The acidity of the modified catalyst was greatly work materials and their derivatives offer new ideas for
improved; the amounts of BASs and LASs in the modified catalyst were high-performance CO2 desorption catalysts. However, there is still a
9.878 and 59.457 μmol/g, respectively (Table 7). Compared with those relative lack of research on MOFs, COFs, and their derivatives, and the
under Ce-MOF catalytic conditions, for CeM–HPW, the CO2 desorption main issue limiting their development is their high cost in industrial
amount and desorption rate were 14% and 54% higher, respectively, application compared with the cost of common catalysts such as metal
and the heat duty for MEA regeneration was 19.7% lower. These en­ oxides and molecular sieves. Therefore, the industrial application of
hancements were due to the synergy between CeO2 and HPW. As illus­ these materials can be promoted by reducing the costs of MOFs and
trated in Fig. 7d, HPW donated protons for attacking the N atom and the COFs themselves.
surface carboxyl group of carbamate, resulting in the elongation of the
C–N bond and the release of CO2. Moreover, the terminal atom of 3.6. Carbon-based materials
MEACOO− could accept protons provided by the –OH group on the
surface of CeO2, causing changes in the molecular structure of Carbon-based materials—including porous carbon, graphene, and
MEACOO− and thus facilitating the decomposition of MEACOO− . The carbon nanotubes—are widely used in catalytic reactions due to their
use of two-dimensional (2D) materials, which are characterized by a high specific surface area, abundant functional groups, and positive
high specific surface area and short diffusion path, can effectively synergy with metal atoms (dos Santos et al., 2017; Mahajan and Gupta,
improve the transport of reacting species and accelerate a reaction. The 2020; Qin et al., 2018). Such materials can be used as SACs for the
structural diversity and tunability of MOFs make them ideal for use in desorption of CO2 from amine-rich solutions (Zhao and Quan, 2021).
conjunction with 2D materials. To solve the stability and acidity limi­ Bairq et al. (2020) took advantage of the high surface area, abundant
tations of SACs, Xing et al. (2022) proposed a novel approach based on BASs, tunable textural features, and high stability of a carbon meso­
the use of 2D cobalt–nitrogen-doped carbon nanoflakes (Co–N–C NSs; porous catalyst (CMK-3) and modified it to obtain CMK-3-M materials
Fig. 7e). The catalyst they synthesized had several notable features, (M = MCM-41, SBA-15, or SiO2), of which CMK-3-SiO2 exhibited the
including excellent stability, a superhydrophilic surface, and high highest catalytic performance. At 97 ◦ C, the CO2 desorption rate was
acidity. The 2D structure of the catalyst had well-confined Co–N4 LASs 95%, higher and the regeneration heat duty was 37.41% lower
and –OH BASs, which synergistically disrupted C–N bonds. The CO2 compared with the noncatalyzed reaction. After 10 cycles, the catalyst
desorption rate was 281% higher and the relative heat duty was 58% retained 85% of its catalytic activity. As displayed in Fig. 8, the catalytic
lower under catalytic conditions than under noncatalytic conditions. mechanism of CMK-3-SiO2 involves the semimetal (e.g., Si) attack of the
Moreover, water evaporation was 20.3% lower. After 20 cycles, the nucleophilic part of the oxygen atom in MEACOO− . A proton is trans­
structure of the catalyst remained the same, and its catalytic perfor­ ferred from the oxygen atom to a neighboring nitrogen atom through the
mance was almost unchanged, which proved that the Co–N–C NSs has isomerization process, resulting in stretching and eventual breaking of
favorable stability at high temperature. This study provides an the C–N bond. In a non-MEA absorption system, Li et al. (2019) inves­
energy-efficient approach to CCS and a comprehensive understanding of tigated the CO2 desorption process in the aqueous solution of
the catalytic process involved. The insights gained from this research 2-(2-aminoethylamino) ethanol and tested the effects of various multi­
can guide the future development of novel nanomaterials. The covalent walled carbon nanotubes—MWCNT, MWCNT-OH, and
bonds in COFs mean that they provide efficient binding sites, and that MWCNT-COOH—as catalysts. When using only 0.05 wt% of these

Table 7
Catalytic desorption properties of organic framework materials and their derivatives.
Catalyst Desorption Des. Rate Des. Amount Relative heat Recyclability Acid site B/L Ref.
temperature (◦ C) increment increment duty (μmol/g)

Non-catalyst – 0% 0% 100% – – –
SZC@TiO2 88 153% 64.5% 64% The catalytic performance had decreased by 0.843/4.084 Xing et al.
approximately 17% after 10 cycles (2021a)
Fe3O4@UiO66- 88 – 80.9% 55.3% 9% loss after 5 cycles – Alivand et al.
SO4 (2022)
CeM-HPW-15 88 166% 38.1% 70.6% 5.1% lower than before the recycling. 9.878/59.457 Wei et al.
(2022a)
Co–N–C NSs 88 281% 83.5% 58% Negligible decrease in catalytic performance 8.530/68.278 Xing et al.
after 20 cycles (2022b)
Ni/Fe@COF 88 114% 30% 42.45% 70.4% of catalytic activity is retained after 4 2.08/25.11 Li et al.
cycles. (2022c)

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S. An et al. Gas Science and Engineering 120 (2023) 205152

Fig. 8. Mechanism of CMK-3 catalytic MEA regeneration. Copyright ACS 2020; Bairq et al., 2020).

catalysts, the CO2 desorption rate was enhanced by 26.7%, 32.4%, and loaded onto catalysts. The specific surface properties of solid catalyst
29.5%. The work of Li et al. provides a reference for the application of materials have a crucial influence on their catalytic activity (Sun et al.,
carbon-based materials for catalytic MEA regeneration. 2023). N2 isothermal adsorption–desorption tests can reveal the specific
Carbon-based materials have proven to have great catalytic potential surface area and pore structure of a catalyst, which are calculated using
for amine regeneration in CCS and are promising candidates for catalytic the Brunauer–Emmett–Teller equation and Barrett–Joyner–Halenda
CO2 desorption. However, the molecular structure of their active centers model, respectively. The surface chemical structure and types of organic
and the specific doping effect that governs the catalytic desorption re­ functional catalysts can be determined using Fourier transform infrared
action are not yet fully understood. Therefore, reports on the catalytic spectroscopy (FT-IR), the results of which have important significance
amine regeneration of carbon-based catalysts remain limited (Pan et al., for guiding the further investigation of a catalyst’s acid center mecha­
2022). nism and reaction mechanism (Guo et al., 2023). Acidity is one of the
In addition, catalytic activity and stability can be improved through most important indexes for evaluating SACs. Py-IR can be used to
doping with nonmetallic atoms (N, S, P, etc.; (Long et al., 2018; Zhang directly and accurately characterize the acid type, acid strength, and
et al., 2016) and constructing metal–carbon composites around acid content of a catalyst. After adsorption of pyridine, the infrared
carbon-based materials as well as single atoms with maximum atomic spectral peak near 1450 cm− 1 is generally attributed to Lewis acidic sites
availability (Pei et al., 2018). (L-acids) of the catalytic material, whereas the infrared spectral peak
near 1540 cm− 1 is attributed to Brønsted acidic sites (B-acids). The
spectral peak at 1490 cm− 1 is the result of the combined action of L-acids
3.7. Summary of SAC analysis methods and B-acids (Zhang et al., 2020c). NH3-TPD is usually combined with
Py-IR to analyze the acid properties of catalysts. Py-IR can be used to
Various characterization methods have been employed to analyze measured different acid types and their corresponding strengths,
SACs in terms of their surface morphology and crystal structure, the whereas NH3-TPD is applied for the comparison of the content of strong
chemical composition and properties of their surface elements, their versus weak acids. As a scattering spectroscopy, laser Raman spectros­
redox properties, and their thermal stability (Yurdakal et al., 2019). copy is useful for characterizing the surface characteristics of materials
X-ray diffraction (XRD) is commonly used for investigating the crystal and can be complementary with FT-IR and XRD (Xing et al., 2020b).
composition, crystallinity, and cell parameters of catalyst materials. Thermogravimetric differential scanning calorimetry is employed to
X-ray photoelectron spectroscopy has been used to characterize the analyze the thermal stability and thermal decomposition behavior of
content, valence state, and proportional distribution of metal ions

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catalysts at high temperature. Inductively coupled plasma atomic the design and screening of desired SACs is currently limited by the
emission spectroscopy can be used to determine the content of metal following bottleneck problems: (1) The structure and composition of
elements in catalysts. Finally, the microscopic morphology of a catalyst catalysts can vary by tens of millions, and relying solely on experimental
material can be examined using field-emission scanning electron mi­ exploration is impossible; (2) The relationship between SACs properties
croscopy (SEM) and high-resolution transmission electron microscopy and target performances (e.g., CO2 desorption amount) are often com­
(TEM) (Ali Saleh Bairq et al., 2019). plex and nonlinear. As a result, elucidating the relationship between
them based on theoretical calculations and/or experiments is often
4. Summary and comparison of SACs’ catalytic desorption complicated, expensive, and time-consuming. Thus, more efficient
activity and stability strategies should be explored in the future to shorten the time required
to discover ideal SACs.
To further guide the industrial application of SACs, we compare and In recent years, machine learning (ML) algorithms have received
analyze the catalytic activity and stability of the six main types of SAC; increased attention in the fields of environment, materials, chemistry,
these are the two most important aspects of catalyst performance. Cat­ etc. Because of their powerful ability to model and predict the complex
alytic activity comprises three indicators—the CO2 desorption rate, and nonlinear relationship between dependent and independent vari­
desorption capacity, and relative heat duty—which indicate the pro­ ables (Zhong et al., 2021). It is a method that uses sample data (i.e.,
portion of improvement relative to noncatalytic conditions. Figs. 9 and training set) to train a model, and then uses the model to predict or make
10 illustrate a positive correlation between the CO2 desorption rate and decisions without relying on certain coding instructions (Zhong et al.,
amount of desorbed CO2. The catalytic performance of unmodified 2021). Common ML algorithms include artificial neural network (ANN),
single-metal oxides, molecular sieves, and natural clay materials is random forest (RF), support vector regression (SVR), eXtreme gradient
generally low, and these catalysts have a limited impact on the CO2 boosting (XGBoost) models and so forth (Yu et al., 2022). ML algorithm
desorption process. Organic framework derivatives and composites have is versatile, which can be used for the prediction, identification of the
outstanding advantages in terms of CO2 desorption kinetics. importance of features, anomaly monitoring, discovery of new materials
Comprehensive comparison of the aforementioned properties in­ or chemicals, etc. (Zhong et al., 2021; Wang et al., 2023b). Although ML
dicates that metal oxide–molecular sieve/natural clay composites and has not been rarely used for CO2 desorption to date, it has shown a
organic framework materials exhibit the highest catalytic ability. These powerful role in CO2 absorption and adsorption and other catalytic
materials also have competent cyclic stability in MEA solution. Notably, systems (Mai et al., 2022; Venkatraman and Alsberg, 2017; Yu et al.,
addition of Fe-Mont and 1/2-SnO2/ATP increased the CO2 desorption 2022; Yuan et al., 2021; Zhong et al., 2021). For example, Yuan et al.
rate by 164%–265% and reduced the relative heat duty to approxi­ (2021) applied ML to reveal the relationship of the textual and
mately 50%. These inexpensive natural-clay-based composites are an compositional properties of biomass waste-derived porous carbons
opportunity for industrial catalytic CO2 desorption technology. More­ (BWDPCs) and adsorption parameters and CO2 adsorption. Results show
over, use of Co–N–C NSs and Fe3O4@UiO-66-SO4 increased the amount that gradient boosting decision trees (GBDTs) exhibited the best pre­
of desorbed CO2 by approximately 80% and reduced the relative heat dictive performance. Further feature importance illustrated that the
duty to lower than 60%. These catalysts also exhibited good stability significance of influencing factors follows the order of adsorption pa­
after more than 10 recycles. rameters (62%) > textural properties (27%) > compositional properties
(11%) for CO2 adsorption on BWDPCs. Shen et al. (2023) employed ML
5. Application prospect of machine learning in CO2 desorption to screen promising phase change solvents via exploring the relationship
process between activator properties and absorption performance. Assessment
results indicated that four phase change solvents with high absorption
Based on the above discussion, fast screening of SACs with high ac­ capacity and low energy penalty were screened based on the relation­
tivity, low cost and strong stability simultaneously is the key to the in­ ship between the physicochemical properties of activators and their
dustrial advances of efficient and low-energy CO2 desorption. However, absorption performances. These results were further verified by the

Fig. 9. Comparison of CO2 desorption performance of different SACs.

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S. An et al. Gas Science and Engineering 120 (2023) 205152

Fig. 10. Cyclic stability of different SACs.

experiments and their kinetics and thermodynamics were superior to as catalyst poisoning and absorbent deactivation mechanisms is
those of benchmark MEA. Li et al. (2023) used ML combined with DFT essential in future studies.
calculations and experiments to reveal that oxidation state of the surface (2) Introduction of ML algorithms combined with experiments and/
Cu active site plays an important role in the selectivity of CO2 electro­ or theoretical calculations to assist in the reasonable design and
reduction reaction (CRR) to C2+ products on oxidized Cu-based cata­ rapid development of catalysts (e.g., the prediction model fabri­
lysts, and the critical potential condition for oxidation state transitions cation, revealing the structure-activity relationships and discov­
from +0 to +0.5 is a reliable descriptor for C2+ selectivity. This finding ery of new SACs and optimization) would significantly facilitate
will benefit researchers in the design of electroreduction conversions of the realization of the efficient and low-energy CO2 desorption in
CO2 to multicarbon C2+ products. In view of this, the introduction of ML the near future.
into CO2 desorption process would be a promising direction and could (3) For the third generation of novel biphasic absorbents, the
well address the two thorny issues mentioned above. Undoubtedly, it coupling process of phase change absorption–catalytic desorption
can promote the industrial progress of CO2 desorption, thus helping to should be investigated to clarify the catalytic desorption mech­
achieve the ambitious goal of “dual carbon". anism and the effect of SACs on phase-change behavior.
(4) Finally, the highly active and stable catalysts developed in recent
6. Conclusion and prospects research remain at the laboratory stage, and the costs of applying
them industrially would be high. Therefore, low-cost carriers
This work highlights the latest progress in catalytic technology for need to be urgently introduced to reduce the cost of existing
desorbing CO2 from amine-rich liquid, mainly covering six types of SAC catalysts, and a catalyst-forming process should be established to
and their catalytic desorption mechanism, catalytic performance, and provide technical solutions for industrial applications. Further­
stability. The future direction of SAC development is presented in more, it remains necessary to screen and select efficient and
accordance with the catalysts’ advantages and disadvantages. Overall, recyclable industrial catalysts suitable for existing decarbon­
inexpensive metal oxide–molecular sieve/natural clay composite ma­ ization processes by conducting small-scale and pilot testing. This
terials are undoubtedly one of the most promising materials for large- is particularly important for catalysts with industrial prospects
scale industrial production and application. Organic framework mate­ such as metal oxide–molecular sieve/natural clay composite
rials and derivatives also have considerable potential, but they are materials (e.g., Fe-Mont and 1/2-SnO2/ATP).
expensive to prepare, which is the critical factor restricting their
development. This study suggests that future research start from the CRediT authorship contribution statement
following points.
Shanlong An: Conceptualization, Validation, Formal analysis,
(1) Under actual working conditions, the types of CO2 absorption Writing – original draft. Teng Xu: Conceptualization, Validation,
products and regeneration pathways are complex, and the cata­ Formal analysis, Writing – original draft. Lei Xing: Writing – review &
lytic regeneration mechanism remains unclear. Moreover, editing. Guanfei Yu: Writing – review & editing. Rongzhe Zhang:
research on the thermal degradation characteristics of absorbents Validation, Data curation. Jingwen Liu: Validation, Data curation.
under catalytic conditions is currently lacking. In addition, cat­ Aizimaitijiang Aierken: Validation, Data curation. Qin Dai: Project
alysts can be deactivated in high-temperature alkaline environ­ administration, Funding acquisition, Writing – review & editing. Lidong
ments. Therefore, addressing challenges related to product Wang: Project administration, Funding acquisition, Resources.
regeneration speed control and enhancement mechanisms as well

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S. An et al. Gas Science and Engineering 120 (2023) 205152

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Chen, Z., Yuan, B., Zhan, G., Li, Y., Li, J., Chen, J., et al., 2022b. Energy-efficient biphasic
To accomplish this work, the authors would like to gratefully solvents for industrial carbon capture: role of physical solvents on CO2 absorption
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22276051), China Postdoctoral Science Foundation (2022TQ0175), the 201–208.
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