Carbon Capture From Flue Gas and The Atmosphere: A Perspective

REVIEW
published: 15 December 2020

doi: 10.3389/fenrg.2020.560849
Carbon Capture From Flue Gas and

the Atmosphere: A Perspective
Xiaoxing Wang 1* and Chunshan Song 1,2,3*
1
PSU-DUT Joint Center for Energy Research, Clean Fuels and Catalysis Program, EMS Energy Institute and Department of
Energy and Mineral Engineering, The Pennsylvania State University, University Park, PA, United States, 2Department of Chemical
Engineering, The Pennsylvania State University, University Park, PA, United States, 3Department of Chemistry, Faculty of Science,
The Chinese University of Hong Kong, Hong Kong, China
Climate change has become a worldwide concern with the rapid rise of the atmospheric
CO2 concentration. To mitigate CO2 emissions, the research and development efforts in
CO2 capture and separation both from the stationary sources with high CO2
concentrations (e.g., coal-fired power plant flue gas) and directly from the atmosphere
have grown significantly. Much progress has been achieved, especially within the last
twenty years. In this perspective, we first briefly review the current status of carbon capture
technologies including absorption, adsorption, membrane, biological capture, and
cryogenic separation, and compare their advantages and disadvantages. Then, we
focus mainly on the recent advances in the absorption, adsorption, and membrane
Edited by:
Michele Aresta,
technologies. Even though numerous optimizations in materials and processes have
IC2R srl, Italy been pursued, implementing a single separation process is still quite energy-intensive
Reviewed by: or costly. To address the challenges, we provide our perspectives on future directions of
Ali A. Rownaghi, CO2 capture research and development, that is, the combination of flue gas recycling and
Missouri University of Science and
Technology, United States hybrid capture system, and one-step integrated CO2 capture and conversion system, as
Wei Wei, they have the potential to overcome the technical bottlenecks of single capture
Shanghai Advanced Research
Institute (CAS), China
technologies, offering significant improvement in energy efficiency and cost-effectiveness.
*Correspondence: Keywords: carbon dioxide capture, flue gas, air capture, hybrid system, carbon capture and conversion
Xiaoxing Wang
[email protected]
Chunshan Song INTRODUCTION
[email protected]
Today’s primary energy supply is heavily relying on carbonaceous fuels, mainly the three typical
Specialty section: fossil energies, that is, coal, petroleum, and conventional and unconventional natural gas. The
This article was submitted to control of pollutants emitted from combustion of these fuels in various stationaries including power
Carbon Capture, Storage, plants, mobile energy systems, and industrial factories is a major challenge to the environment and
and Utilization, human health and safety. It is initially related to the emissions of SOx, NOx, mercury, and particulate
a section of the journal
matters. Now, it also involves the emissions of carbon dioxide (CO2) and methane (CH4), two major
Frontiers in Energy Research
greenhouse gases which have been regarded as the main reason for the climate change worldwide.
Received: 10 May 2020
With increasing concerns on global climate change (Melillo et al., 1993; Houghton et al., 2001; IPCC,
Accepted: 22 September 2020
2015), reducing greenhouse gases emissions, particularly CO2 emissions, has been significantly
Published: 15 December 2020
heightened in both academia and industry in recent years (Maroto-Valer et al., 2002; Brovkin et al.,
Citation:
2004; Song, 2006), in part because the increased CO2 emissions are believed to contributing to ocean
Wang X and Song C (2020) Carbon
Capture From Flue Gas and the
acidification and sea level rise in addition to global warming and climate change.
Atmosphere: A Perspective. Since the industrial revolution, CO2 emissions have increased continuously due mainly to the
Front. Energy Res. 8:560849. anthropogenic activities. Figure 1 shows the CO2 concentration in the atmosphere within the last six
doi: 10.3389/fenrg.2020.560849 decades from 1958 to 2019. As of December 2019, CO2 concentration in the atmosphere has reached
Frontiers in Energy Research | www.frontiersin.org 1 December 2020 | Volume 8 | Article 560849

Wang and Song A Perspective on CO2 Capture
FIGURE 1 | Atmospheric CO2 concentration during 1950–2019 (data sources: http://climate.nasa.gov/vital-signs/carbon-dioxide/).
412 ppm, accounting for about 31% increase of that in 1958 2009; Lackner et al., 2012; IPCC, 2015; Sanz-Pérez et al., 2016;
(∼5.1‰ per year). In contrast, it took about a hundred years for National Academies of Sciences, Engineering, and Medicine, 2019).
the atmospheric CO2 concentration to reach 315 ppm by 1958 There are several pathways to mitigate CO2 emissions:
(IPCC, 2015; Seneviratne et al., 2016), an increase of ∼12.5% reducing energy use, improving energy efficiency, shifting to
(∼1.25‰ per year). Such a change clearly shows that the low-carbon or even non-carbon energy, and implementing
atmospheric CO2 concentration has increased significantly, and carbon capture and sequestration (CCS) (Pacala and Socolow,
the rising rate becomes faster and faster. The CO2 concentration 2004). Reducing energy use is not realistic on a global scale, while
in air would surpass 550 ppm by 2050 if no action were taken to curb improving energy efficiency is a highly challenging task to meet
CO2 emissions while keeping fossil fuels utilization as is (Smith and the climate change mitigation goals. The use of low-carbon
Myers, 2018), possibly reaching to 900–1,100 ppm by the end of this energy such as natural gas can slow but not be able to solve
century (Kiehl, 2011). If so, it could cause catastrophic impact on the problem. Renewable energy such as biomass, wind, and solar
global climate and human nutrition and societies. is still at its early stage and not able to replace the current fossil
In 2015, a global agreement was reached at the United Nations fuel-based energy in near future, while the future of nuclear
Climate Change Conference, known as the Paris Agreement. It energy is under much debating with big uncertainty. In contrast,
sets a target of keeping the global temperature rise at 2°C or less by carbon capture, utilization, and sequestration (CCUS), which
the end of the 21st century (United Nations Climate Change, refers to a process that captures CO2 from sources like power
2015), accentuating well on the urgency in reducing CO2 plants or ambient air followed by recycling it for utilization or
emissions (Seneviratne et al., 2016). However, with fast growth sequestrating it underground permanently, is now widely
of global economies and world population which demands more regarded as a viable option to quickly alleviate CO2 emissions
and more energy supply globally, fossil fuels will continue playing within a midterm. Especially, when the captured CO2 is utilized as
a major role. Although the supply of alternative energies such as a valuable (and renewable) feedstock and cheap carbon source for
biomass, solar, and wind is increasing, they are still in the industrial chemicals and fuels production, it offers a cost-
developing stage, yet far from ready to replace the fossil competitive way to solve the contradict between the ever-
energy completely. Thus, developing strategies to significantly increasing energy demand and CO2 emissions reduction
reduce CO2 emissions both from the stationary sources with high (Markewitz et al., 2012).
CO2 concentrations (e.g., coal-fired power plants, and Today, the global energy-related CO2 emissions are at the
manufacturing industries) and directly from air have attracted level of 35–37 gigatonnes per year (Gt/yr), with over 80%
increasing attention worldwide (Lackner, 2003; Song, 2006; Keith, coming from fossil fuel combustion--> (National Academies

of Sciences, Engineering, and Medicine, 2019; IEA, 2010; CURRENT STATUS OF CARBON CAPTURE
OECD, 2012). In the United States, the energy-related CO2 TECHNOLOGIES
emissions are about 5.1–5.3 Gt/yr in recent years (U.S. Energy
Information Administration, 2020). Among them, the CO2 Currently, several technological pathways are pursued for CO2
emissions from power plants, industrial sector, and the separation and capture including carbon capture from post-
transportation sector account for 30, 21, and 26% of total combustion, pre-combustion, oxy-combustion, chemical
carbon emissions, respectively (United States Environmental looping combustion (CLC), and ambient air as well, which is
Protection Agency, 2016). Capturing CO2 from these sources is illustrated in Figure 2. Table 1 lists the advantages and
thus critical to maintain or slow down the increase of the disadvantages of those pathways (Figueroa et al., 2008;
atmospheric CO2 level (Sanz-Pérez et al., 2016). About Rackley, 2017).
1.3 Gt-CO2 is emitted annually from the transportation
sector in the United States, which is expected to increase • Post-combustion capture involves CO2 separation from flue
significantly by 2050 due to the increasing demand for gases after combustion, which has a low CO2 partial
vehicles and aviation (OECD, 2012). Unfortunately, till pressure (0.03–0.2 bar) and/or a low CO2 concentration
today, onboard CO2 capture from the mobile system is still (3–20%) (Figueroa et al., 2008; Feron and Hendriks,
not available. To address the challenge, negative emission 2005). The carbon capture from some industrial sources
strategies have recently been proposed. One method is such as cement manufacturing, stainless steel factory can
directly removing CO2 from air, the so-called direct air also be categorized into post-combustion capture, although
carbon capture (DACC) (Keith, 2009; Lackner et al., 2012; the CO2 concentration from those industrial processes is
Sanz-Pérez et al., 2016; National Academies of Sciences, higher than that of a typical flue gas from post-combustion
Engineering, and Medicine, 2019). According to the power plants. Table 2 lists the typical CO2 concentration of
Intergovernmental Panel on Climate Change (IPCC), the a flue gas stream from various sources (Metz et al., 2005;
current global CO2 emissions are more than those envisaged Husebye et al., 2012; Liguori and Wilcox, 2018). The
with the most pessimistic model (Stocker et al., 2013). Thus, commercially available post-combustion capture process
combining CO2 capture both from the high and low CO2 is the chemical absorption-based aqueous amine solution,
concentration sources could be essential to achieve the Paris such as 30% monoethanolamine (MEA) solution. Post-
Agreement goal of limiting anthropogenic global temperature combustion capture is considered as a more viable option
increase below 2°C. for existing coal-fired power plants (Wang Y. et al., 2017).
Aqueous amine scrubbing is the benchmark carbon capture • In a pre-combustion process, which is based on the scaled
technology currently commercially available in industry industrial processes for the production of hydrogen and
(Rochelle, 2009; Rochelle, 2016; Tontiwachwuthikul and Idem, chemical commodities (Jansen et al., 2015), fuel feedstocks
2013; Darunte et al., 2016). This process, however, is very energy (i.e., coal and natural gas) are converted into syngas (H2 and
intensive. It is predicted that the required parasitic loads or the so- CO) via gasification, steam reforming, auto thermal
called energy penalty for CO2 removal is around 0.2–0.5 MWh/ reforming, or partial oxidation (Steinberg and Cheng,
ton-CO2, which is equivalent to 20–30% of power plant output 1989), and then CO is transferred into CO2 by water,
(Rochelle, 2009). Particularly, the absorbent regeneration and with more hydrogen produced (the so-called water–gas
CO2 recovery step consumes about 50% of the overall energy in shift reaction, WGS), followed by carbon capture system
the form of low-pressure steam for the stripper reboiler due to remove CO2. After CO2 is captured, the hydrogen-rich
largely to the high heating capacity of water. The high energy fuel gas is utilized for power and heat generation such as
penalty induces both high capital cost and operating cost. The use boilers, gas turbines, and fuel cells (Metz et al., 2005). After
of basic amine solution can cause corrosion to the equipment. WGS, the CO2 concentration in the flue gas is relatively
Furthermore, the amine loss due to the degradation and high, which is in the range of 15–60% (dry basis) at a total
evaporation in the process generates pollutants to the pressure of 2–7 MPa (Gazzani et al., 2013a; Gazzani et al.,
environment. It is estimated that the application of the 2013b), thus physical solvents such as Selexol and Rectisol
technology could result in the increase in the cost of electricity rather than chemical solvents are commonly used for pre-
by 25–40% (Rubin et al., 2015), thus limiting its widespread use combustion capture.
(Haszeldine, 2009). Therefore, developing new technologies to • Oxy-combustion is a relatively new technology (Jurado
minimize energy penalty and improve cost-effectiveness for et al., 2015) and involves the combustion of fuel
carbon capture is highly desired yet quite challenging (Song, feedstocks in a nearly pure oxygen (95–99%) or
2006; Chu, 2009; Keith, 2009). In this article, we first convey a O2–CO2–rich environment (Miller, 2017), resulting in a
short review on the R&D status of carbon capture technologies flue gas with very high CO2 concentration, where the
including absorption, adsorption, membrane, biological capture, capture of CO2 is thus normally not needed and CO2 is
and cryogenic separation; compare their advantages and basically ready for sequestration (Miller, 2017; Li et al., 2018;
disadvantages; and elaborate mainly on absorption, adsorption, Wu et al., 2019). However, in order to obtain nearly pure
and membrane technologies more in detail. Then, we provide our oxygen (>95%) (Kather et al., 2008), usually a cryogenic air
perspective on future directions in CO2 capture research and separation unit is required for oxygen separation from air,
development. which makes the whole process costly.

FIGURE 2 | Schematic diagram of the existing CO2 capture pathways.
• CLC is an emerging combustion process similar to oxy- the oxygen carrier plays a critical role in the chemical
combustion producing the CO2-concentrated flue gas looping process. More recently, the machine learning
(Abanades et al., 2015; Miller, 2017), so that the algorithms and artificial neural networks have been
separation of CO2 from fuel gas (e.g., pre-combustion) or utilized to estimate the performance of hetero- and
flue gas (e.g., post-combustion) is not needed. In a typical multi-component materials as oxygen carriers for CLC
chemical looping process, an oxygen carrier such as Fe, Mn, (Yan et al., 2020).
Cu, Ni, and Co metals is oxidized in air in one reactor (called • DACC represents a process for CO2 extraction or removal
the air-reactor), which is then reduced with a hydrocarbon directly from the atmosphere, which was first introduced for
fuel in another reactor (called the fuel-reactor) to regenerate the mitigation of climate change by Lackner in 1999
the metal and release CO2 and water (Abanades et al., 2015). (Lackner et al., 1999). DACC could play a crucial role for
The metal is then sent back to start another cycle in the air- CO2 capture from decentralized and mobile emission
and fuel-reactors. The exothermic air-reactor provides sources such as vehicles, ships, or air planes (Sanz-Pérez
higher temperature heat and power, while the fuel- et al., 2016; Bhown et al., 2020; Jones, 2011; Goeppert et al.,
reactor can also generate some heat and power as well. 2012), thus gaining increasing attention. In 2012, Kulkarni
CLC was introduced first by Lewis et al. (Lewis et al., 1951) and Sholl (Kulkarni and Sholl, 2012) developed a steam-
and later applied for CO2 mitigation by Ishida et al. (Ishida based process using aminosilica sorbents, which can recover
et al., 1987; Ishida and Jin, 1994). Since then over 900 CO2 at 1–3 ton/unit/year. Currently, multiple companies
materials have been tested (Lyngfelt and Mattisson, 2011) including Carbon Engineering (Carbon Engineering, 2020),
and a number of reviews have been published (Fan, 2010; Climeworks (Climeworks, 2020), and Global Thermostat
Adanez et al., 2012; Lyngfelt, 2014; Abanades et al., 2015). (Global Thermostat, 2020) are developing DACC systems at
Compared to oxy-combustion, CLC eliminates the costly air a commercial scale. However, it is quite challenging due to
separation unit, thus is more cost-effective, but the process is the exceptionally low CO2 concentration (∼400 ppm in air).
relatively more complicated, requiring more studies. To be It requires moving very large volume of air through the
more cost competitive, a suitable metal/metal–oxide pair as capture unit and high adsorption heat to execute the CO2

extraction, making this pathway more energy intensive and
• Costly and energy intensive due to extremely low CO2 concentration (∼400 ppm)
costly than removing CO2 from the concentrated sources.
There is a debate on whether DACC is an enabling factor
(Realmonte et al., 2019; Azarabadi and Lackner, 2020) or
just a costly distraction for effective climate change
mitigation (Chatterjee and Huang, 2020).
• H2-rich gas-induced temperature and efficiency issues

Other industrial processes such as hydrogen production,
• Retrofit unattractive due to Significant plant changes

ammonia synthesis, and methanol manufacture release the tail
• Costly and energy intensive air separation step

• Low capture efficiency due to low CO2 partial
gases with a high concentration of CO2, which could be captured

Cons
and directly used or transported for storage after some
• Immature, currently under development
• Immature, currently under development

• Applicable mainly to new IGCC plants
purification. Similar to the oxy-combustion and CLC

processes, an individual CO2 capture unit is normally not
✓Mature technology (e.g., aqueous monoethanolamine (MEA)), commercially deployed in some industries • High parasitic power requirement
• High capital and operating costs
needed for those processes.

As shown in Figure 2, only post-combustion capture, pre-
combustion capture and air capture require a CO2 capture
system. So far, many technological approaches are available for
a carbon capture system; however, the choice of a specific capture
technology differs widely depending on the sources and CO2-
generating processes, resulting in different energy penalties.
pressure
in air
Figure 3 illustrates various CO2 capture technologies including

absorption, adsorption, membrane, biological capture, and
cryogenic capture under investigation in both academia and
✓Mature physical absorption technology (e.g., Selexol and Recticol), commercially deployed in some
industry for the past few decades, while Table 3 briefly

compares the advantages and limitations of these carbon
capture technologies (Singh and Dhar, 2019). Among them,
absorption, adsorption, and membrane methods are more
intensively studied, thus are further discussed in the following
section.
✓Viable alternative for CO2 capture from mobile and decentralized sources
Absorption
Among the abovementioned CO2 capture options, the technology
based on liquid absorption is most mature and commercially
✓Truly and directly reduce the atmospheric CO2 concentration
available, especially in the petroleum and chemical industries.

industries,
Based on the nature of the interaction between the absorbent and

✓Possible for retrofit and repowering to existing plants
Pros
CO2, it separates as chemical absorption (mainly applied for CO2

capture from post-combustion flue gas) and physical absorption
✓Developed air separation technologies available
TABLE 1 | Pros and cons of current CO2 capture technological approaches.
(mainly used for CO2 capture from pre-combustion flue gas).

Aqueous amine solutions (e.g., 20–30 wt% MEA, and
✓Good for most existing power plants
✓Possible for retrofit to existing plants
diethanolamine (DEA)) and liquid ammonia are typical

✓Low cost oxygen carrier materials
solvents for chemical absorption. MEA solution has become

✓Very high CO2 concentration
✓Very high CO2 concentration
the benchmark amine for CO2 capture from power plants

because it has good CO2 transfer rates, relatively low cost, and
✓High CO2 concentration
✓High partial pressure
biodegradable. However, it suffers from toxicity and solvent loss

due to evaporation and degradation (Bui et al., 2018). In addition,
at higher concentrations, MEA solution is highly corrosive to the
equipment.
Developing new CO2 absorbents to replace MEA has thus
aroused much interests and is still ongoing. Normally, thermal
swing absorption–regeneration is used for chemical absorption;
thus, selecting an absorbent with optimized thermal and physical
properties is crucial to the development of energy-efficient and
Oxyfuel combustion
Capture pathway
cost-effective carbon capture absorption technology. So far, a

Chemical looping
Post-combustion
Pre-combustion
large number of solvents, including single amines, amine blends,

combustion
Air capture
and amino acids, have been evaluated individually for their

performance in CO2 capture (Bui et al., 2018; Sreedhar et al.,
2017). Figure 4 shows the CO2 absorption capacities in mol-CO2

TABLE 2 | Typical CO2 concentration of a flue gas from various sources (Metz et al., 2005; Husebye et al., 2012; Liguori and Wilcox, 2018).
Flue gas source CO2 conc. (%) P (atm) CO2

partial pressure (atm)
Gas turbine 3–4 1 0.03–0.04

Fired boiler of oil refinery and petrochemical plant ∼8 1 0.08
Natural gas fired boilers 7–10 1 0.07–0.10
Oil-fired boilers 11–13 1 0.11–0.13
Coal-fired boilers 12–14 1 0.12–0.14
IGCCa after combustion 12–14 1 0.12–0.14
Hydrogen production 15–20 22–27 3–5
Steel production (blast furnace) 20–27 1–3 0.2–06
Aluminum production 1–2 1 0.01–0.02
Cement process 14–33 1 0.14–0.33
a
IGCC, integrated gasification combined cycle. Data extracted from the literature (Figueroa et al., 2008; Chu, 2009).
FIGURE 3 | Illustration of various CO2 capture technologies along with typical materials currently under investigation.
per mol-amine obtained at 40°C and CO2 partial pressure of Rochelle, 2011; Rebolledo-Morales et al., 2011; Schäffer et al.,
15 kPa using different amines with different structures at 2012; Tong et al., 2012; Chang et al., 2013; Monteiro et al., 2013;
different amine concentrations (Shen and Li, 1992; Jou et al., Yamada et al., 2013; Arshad et al., 2014; Bougie and Iliuta, 2014;
1995; Park et al., 2002; Benamor and Aroua, 2005; Derks et al., Li et al., 2014; Li and Rochelle, 2014; Nouacer et al., 2014; Chen S.
2005; Maneeintr et al., 2009; Puxty et al., 2009; Chen and et al., 2015; Conway et al., 2015; Mondal et al., 2015; El Hadri

Frontiers in Energy Research | www.frontiersin.org
Wang and Song

TABLE 3 | Comparison of typical CO2 capture technologies.
Technology Mechanisms Pros Cons
Absorption Chemical absorption (e.g., MEA and chemical reaction between a solvent and CO2 ✓High capacity at low CO2 pressure • Energy-intensive regeneration
NaOH) ✓Mature technology • Low absorption–desorption rate
• Corrosion
• Absorbent degradation
• High operating cost
Physical absorption (e.g.,methanol, The solubility of CO2 in a solvent ✓High capacity at low temperature and • Low selectivity
Selexol, and Rectisol) high pressure • High energy consumption
✓Cheaper solvent • Low capacity at high temperature and low pressure
✓Mature technology • Absorbent loss
Adsorption Physical adsorbents (e.g., AC, Molecular sieve confinement effect of solid ✓High capacity at low temperature and • Low CO2 selectivity
zeolites, and MOF) materials, normally with micropores high pressure • Capacity decreases with temperature
✓Low waste generation • Normally require high pressure
• Moisture degrades the adsorbent performance
Chemical adsorbents (e.g., CaO and Through the formation of carbonates or ✓Work at high temperature • Require high temperature for CO2 sorption and adsorbent regeneration
Na2SiO3) bicarbonates ✓High capacity
— — • High energy consumption
✓Low waste generation • Performance loss with cycles
Solid amine sorbents (e.g., PEI/SiO2) Chemical reaction between amine groups and ✓High capacity at low CO2 pressure • Thermal and oxidative degradation
7
CO2 ✓High selectivity • Degradation due to contaminants (e.g., SOx and NOx)
✓Fast kinetics
✓Mild conditions
✓Positive effect of moisture
✓Lower energy consumption
✓Less corrosion
✓Low waste generation
Membrane Different gas permeability ✓Relatively low operation cost • High manufacturing cost
✓Easy handling and Operation • Relatively low separation selectivity
• Permeability still low
• Negative effect of moisture
Biological absorption/utilization Captured and utilized through photosynthesis in ✓No hazards of chemicals • Long time requirement
• Large area requirement
December 2020 | Volume 8 | Article 560849
plants
• May affect biological diversity
✓Coproduction of food, biofuels, and • Sensitive to other flue gas contaminants (e.g., SOx and NOx) and culture
value-added products conditions (pH, temperature, and salinity)
Cryogenic separation Different condensation temperature ✓High capture efficiency (up to 99.9%) • High energy requirement
A Perspective on CO2 Capture

• Low efficiency
• Moisture pre-removal is required
• Solidified CO2 may be accumulated on the surface of heat exchanger
FIGURE 4 | CO2 uptakes obtained at 40°C and CO2 partial pressure of 15 kPa using different liquid amines with different structures at different amine
concentrations. Data from the literature (Shen and Li, 1992; Jou et al., 1995; Park et al., 2002; Benamor and Aroua, 2005; Derks et al., 2005; Maneeintr et al., 2009;
Puxty et al., 2009; Chen and Rochelle, 2011; Rebolledo-Morales et al., 2011; Schäffer et al., 2012; Tong et al., 2012; Chang et al., 2013; Monteiro et al., 2013; Yamada
et al., 2013; Arshad et al., 2014; Bougie and Iliuta, 2014; Li et al., 2014; Li and Rochelle, 2014; Nouacer et al., 2014; Chen S. et al., 2015; Conway et al., 2015;
Mondal et al., 2015; El Hadri et al., 2017).
et al., 2017). The majority were examined at the amine There is another class of amine-based solvents which is called
concentration between 2 and 3.5 mol/L. The CO2 absorption phase-change solvents including amine–alcohol system and
capacity is ranged from 0.4 to 1.4 mol-CO2/mol-amine. More amine–water system. Upon CO2 absorption or increasing the
specifically, for the primary, secondary, and tertiary mines in temperature after CO2 absorption, the solvent divides into two
straight chains, multi-amines, and amines in cyclic chains, their phases: CO2-rich and CO2-lean phases (Zhuang et al., 2016;
capacities are in the range of 0.5–0.7, 0.4–0.8, 0.4–0.9, 0.8–1.4, Papadopoulos et al., 2019). In contrast to traditional solvents,
and 0.5–1.1 mol-CO2/mol-amine, respectively. The CO2 only the CO2-rich phase is sent for regeneration; therefore, the
absorption capacity decreases generally following the amine energy demand and the size of the regenerator can be
structure as cyclic amines ≈ multi-amines > tertiary-amines > dramatically reduced in comparison to non–phase-change
secondary-amines > primary-amines. Among them, piperazine solvents. Gomez et al. compared the performance of phase-
(PZ) absorbent has been suggested as a good alternative to change solvent process to the conventional MEA process,
conventional chemical solvents. Compared to MEA, it shows showing the CO2 capture cost could be saved by 15.4% for the
fast kinetics in reaction with CO2, better chemical stability, and power plant, and as much as 51.7% for the cement plant (Gomez
requires lower energy input for regeneration (Rochelle, 2009; et al., 2014). Although the phase-change absorbent systems
Dugas and Rochelle, 2011). It also exhibits better resistance to exhibit some potential merits and economic incentives for
oxidative and thermal degradation (Freeman et al., 2010a). scaling up, they may be volatile and corrosive due to the use
Other amine blends such as PZ/AMP (Seo and Hong, 2000; of amine solution in nature. The formation of precipitation and
Khan et al., 2016) and K2CO3/PZ (Tim Cullinane et al., 2005; salts is another important issue for the implementation of the
Cullinane and Rochelle, 2006) have also been studied, and it has phase-change solvent-based absorption process.
been found that the blending can improve the absorption Besides the chemisorption using amine solutions, another type
kinetics, thermodynamic efficiency, and resistance to of absorption technology is using physical solvents to absorb CO2,
degradation. The main drawback of PZ is that it could form which is based on their CO2 solubility (Chakma, 1999). Physical
precipitation and nitrosamine during CO2 capture process absorption is generally preferred at higher pressures. Selexol,
(Freeman et al., 2010b; Cousins et al., 2015). Rectisol, Purisol, and Fluor are the well-established commercial

physical absorption technologies, and also energy-intensive selectivity, and impurity tolerance. So far, a large number of solid
processes due to their heat transfer requirements (Figueroa adsorbents have been investigated, including carbons and carbon
et al., 2008). Since the physical absorption is depended on nanotubes (Aaron and Tsouris, 2005; Huang et al., 2007; Plaza
physical interaction rather than chemical reaction, it normally et al., 2007; Razavi et al., 2011), clays and oxides (Ding and Alpay,
requires higher partial pressure of CO2 and is preferred at low 2000; Yong et al., 2001; Gray et al., 2005; Hiyoshi et al., 2005),
temperatures in order to achieve high CO2 capture capacity, microporous zeolites and mesoporous molecular sieves
which thus reduces its efficiency and increases its operation cost. (Takamura et al., 2001; Siriwardane et al., 2003; Son et al.,
Recently, ionic liquids (ILs), which consist of ions and act as liquid 2008; Zelenak et al., 2008a), and microporous metal–organic
at room temperature (Hallett and Welton, 2011), are considered as framework materials (MOFs) (Torrisi et al., 2010; Zhang Z.
suitable alternatives to the traditional physical absorbents, because ILs et al., 2013; Gonzalez-Zamora and Ibrra, 2017).
have unique properties such as low volatility, low vapor pressure, and Zeolites are widely used in refinery and gas separation
good thermal stability (Bates et al., 2002; Corvo et al., 2015; Zeng et al., industry, and have shown high CO2 uptake such as zeolite
2017). In addition, after CO2 absorption, its energy requirement for 13X and Ca-A, reaching about 3 and 3.72 mmol/g, respectively
regeneration is also relatively low. Figure 5 presents the CO2 (Bae et al., 2013). CO2 adsorption over zeolites is derived from the
absorption capacities of some typical ILs (Zhang et al., 2008; Pérez- interaction between the electric field of zeolite and the large
Salado Kamps et al., 2003; Shiflett and Yokozeki, 2005; Shin et al., 2008; quadrupole moment of CO2. Thus, both the structure and
Carvalho et al., 2010; Kilaru and Scovazzo, 2008; Anderson et al., 2007; composition of zeolite framework, and the composition and
Aki et al., 2004; Blanchard et al., 2001). As seen, the CO2 absorption location of cations govern its CO2 adsorption performance
capacity varies with the type of ionic liquid. The highest value of (Grajciar et al., 2012; Kim et al., 2012). Lin et al. screened
0.88 mol-CO2/mol-IL (moles of CO2 per mole of IL) was obtained with over hundreds of thousands of zeolites and zeolitic imidazolate
[THTDP][NTf2] ionic liquid, while the [hmpy][Tf2N] ionic liquid frameworks (ZIFs) via a computational approach and identified
gave the lowest value of 0.20 mol-CO2/mol-IL (Anderson et al., 2007). potential materials for CO2 capture (Lin et al., 2012). The main
The max CO2 solubility in ILs reported in the literature is largely within weakness of zeolites is their sensitivity to moisture, which results
the range of 0.4–0.8 mol-CO2/mol-IL, which is comparable to those of in a significant reduction of CO2 uptake (Bui et al., 2018).
most aqueous amine solutions as shown in Figure 4. However, their MOFs are a relatively new class of crystalline porous materials
high viscosities and relatively low working capacity are the two main constructed via self-assemblage of metal “nodes” and organic
obstacles for their application in CO2 capture. To attain higher CO2 linkers (Long and Yaghi, 2009; Zhou et al., 2012; Lu et al., 2014).
capacity, a series of the so-called task-specific ILs have been designed by MOFs possess very high surface areas and pore volumes.
incorporation of various functionalities, such as carboxylate anions, Theoretically, by varying the metal and the linker, infinite
amine and amino acid groups, or azolates for chemisorption of CO2, different MOFs can be synthesized, and their physicochemical
thereby significantly boosting the absorption capacity up to about properties are consequently tuned in terms of CO2 capacity,
0.5–2.0 mol-CO2/mol-IL under atmospheric pressure (Bates et al., selectivity, and heat of adsorption, which makes them highly
2002; Giernoth, 2010; Wappel et al., 2010; Petkovic et al., 2011; attractive for CO2 capture (Singh et al., 2020). For example,
Shannon and Bara, 2012; Cui et al., 2016). Several groups have also MOF-74(Mg) showed a high CO2 adsorption capacity of
studied the physical and chemical properties of CO2–IL systems using 5.5 mmol/g at 0.15 bar CO2 and 40°C (Caskey et al., 2008; Bae
thermodynamic modeling (Zhang et al., 2008; de Riva et al., 2017), et al., 2013), while UiO-66 and SIFSIX-6_Zn exhibited good
kinetics (Wang C. et al., 2011; Moya et al., 2014; de Riva et al., 2017) and resistance to other flue gas components such as water, SOx,
CO2 sorption mechanisms (Carvalho et al., 2009; Shiflett et al., 2010). and NOx (Nugent et al., 2013; Burtch et al., 2014; Wang C.
Although higher capacity can be obtained, the functionalized ILs show et al., 2016). In a recent article, Ding et al. conducted a
higher viscosities than unfunctionalized ILs. Therefore, how to greatly comprehensive review on MOFs for CO2 capture and
reduce the viscosity while maintaining its high capacity is the largest conversion, where they summarized and compared the
technical challenge for the successful use of ILs in CCS. High cost and reported MOFs for CO2 capture in terms of their CO2
difficulty in scale-up are other two significant barriers to the wide capacities (Ding et al., 2019).
spread of ILs for CCS (Singh and Dhar, 2019). Carbon materials including activated carbons, carbon
nanotubes, and graphene have also been studied for CO2
Adsorption capture due to their low cost and wide availability (Wang Q.
Adsorption is widely deemed as a promising technology for CO2 et al., 2011; Montagnaro et al., 2015; Taheri Najafabadi, 2015;
capture as it can be retrofitted to any power plants, operated at Mohamedali et al., 2016). The capability of carbon materials for
various conditions with relatively high capacity, high CO2 CO2 adsorption mainly relies on its porosity; thus, the higher the
selectivity, and low energy requirement for regeneration. It can pore volume, particularly the micropores, the higher the CO2
be applied for both pre- and post-combustion pathways (Bui capacity (Estevez et al., 2018). Carbons work better at high
et al., 2018). If waste materials are utilized for preparation of pressure. While at low pressure, their CO2 capacities are
adsorbents, the adsorption process could be potentially more typically lower than those of zeolites. Compared to zeolites,
sustainable. It should also be highlighted that adsorption method carbons possess much better stability in the presence of water
is well suited for CO2 capture directly from air. (Xu et al., 2013).
Currently, most efforts in developing advanced adsorbents Another type of solid adsorbents is oxides including CaO,
have been focused on improving CO2 adsorption capacity, CO2 MgO, and FeO (Feng et al., 2007; Florin and Harris, 2009; Mutch

FIGURE 5 | The reported maximum CO2 absorption capacity of some typical ionic liquids for CO2 capture at 40°C with CO2 partial pressure of 15 kPa, data from
the literature (Zhang et al., 2008; Pérez-Salado Kamps et al., 2003; Shiflett and Yokozeki, 2005; Shin et al., 2008; Carvalho et al., 2010; Kilaru and Scovazzo, 2008;
Anderson et al., 2007; Aki et al., 2004; Blanchard et al., 2001).
et al., 2018; Mora Mendoza et al., 2019); layered double tolerance to water with no or less corrosion to the equipment (Ma
hydroxides (LDHs) (Ram Reddy et al., 2006; Ram Reddy et al., 2009; Choi et al., 2009; Wang et al., 2009; Bollini et al., 2011;
et al., 2008); and alkali metal–containing ceramics such as Wang and Song, 2019). By far, three popular approaches are
Li2ZrO3 (Nakagawa, 1998), Li4SiO4 (Gauer and Heschel, proceeding in preparation of those amine-based sorbents, which
2006), and Na2SiO3 (Rodríguez and Pfeiffer, 2008). Those are outlined in Figure 6, including 1) immobilizing amine
adsorbents are normally handled at high temperatures within compounds (e.g., PEI, TEPA, DEA, and dendrimers (Wang
the cyclic carbonation/calcination reactors. High temperature et al., 2005; Yue et al., 2006; Liang et al., 2008; Qi et al.,
(>500°C) causes the sintering of oxides, which results in the 2011)) onto a nanoporous support (Xu et al., 2002; Xu et al.,
dramatic reduction of their CO2 capture performance (Erans 2003; Xu et al., 2005; Ma et al., 2009; Chen et al., 2010; Liu et al.,
et al., 2016). 2010; Tanthana and Chuang, 2010; Wang D. et al., 2011; Zhang
Compared to abovementioned adsorbents, amine-based solid et al., 2012; Yang et al., 2013) and/or microporous zeolites (Kim
sorbents are the center of investigation in adsorption. Since the et al., 2016) and MOFs (Demessence et al., 2009; Lee et al., 2014;
first report on polyethylenimine (PEI)-based sorbents showing McDonald et al., 2015) by a conventional wet impregnation
good performance for CO2 separation, the so-called molecular method; 2) growing reactive amine monomers inside the
basket sorbents (Figure 6) (Xu et al., 2002), in the past twenty porous material via in situ polymerization method or
years, solid sorbents containing amines, have aroused significant incorporating amine compounds with silica precursor during
interests for CO2 capture and later for CO2 removal directly from mesoporous material preparation via co-condensation method
air (Yu et al., 2012). The use of amine-functionalized sorbents can (Tsuda et al., 1992; Tsuda and Fujiwara, 1992; Rosenholm et al.,
greatly reduce the need in the parasitic energy input (mainly 2006; Rosenholm and Linden, 2007; Hicks et al., 2008); and 3)
because solid has lower heat capacity than water), and offer high covalently grafting amine compounds (e.g., (3-aminopropyl)
CO2 capacity and selectivity, fast kinetics, multicycle stability, and trimethoxysilane and (3-aminopropyl)triethoxysilane) on a

FIGURE 6 | Schematic illustration of the widely used three approaches in preparation of the amine-based sorbents.
support surface via post-synthesis method (Huang et al., 2003; To have a better overall picture, the CO2 capacities reported in
Hiyoshi et al., 2004; Hiyoshi et al., 2005; Zelenak et al., 2008b; the literature with different support at different PEI loading and
Belmabkhout and Sayari, 2009; Kumar and Guliants, 2010). sorption temperature for CO2 capture from pure CO2 and the
Polymer PEI contains repeating -CH2CH2-NH-units. Because it simulated air containing ∼400 ppm CO2 are plotted in Figure 7.
has high nitrogen content in mass and relatively good thermal For CO2 capture from pure CO2 (Figure 7A), the higher the PEI
stability (Yue et al., 2008; Goeppert et al., 2011), PEI is often loading, the higher the CO2 uptake. Increasing temperature also
selected for amine-based sorbents, becoming a promising benefits CO2 sorption. Generally, high CO2 capture capacity of
candidate suitable not only for CO2 capture from flue gases with around 150–200 mg/g is mostly reported, which is favored at
relatively high CO2 concentration, but also good for direct air capture. 50–70 wt.% PEI loading at 70–90°C. The amine efficiency (termed
Other amines such as tetraethylenepentamine (TEPA), as A.E.), which is defined as moles of CO2 captured per mole of N
pentaethylenehexamine (PEHA), MEA, DEA, and groups in the sorbent, is presented as an inset in Figure 7A. It
diisopropanolamine are more prone to leaching issue due to their shows the major value of about 0.30 (the black dot line in the inset
relatively low molecular weight and boiling points, which could cause of Figure 7A). It is widely accepted that under dry condition, two
CO2 capacity loss and pollute the downstream equipment of the N sites are needed for one CO2 molecule through the formation of
sorption system (Goeppert et al., 2014). Many reviews on solid- zwitterions. Although tertiary amine does not directly react with
sorbent–based CO2 capture have been published (Song, 2006; Sanz- CO2, it could accept the proton from zwitterions generated by the
Pérez et al., 2016; Darunte et al., 2016; Choi et al., 2009; D’Alessandro reactions between CO2 and primary/secondary amines,
et al., 2010; Lin et al., 2016; Didas et al., 2015; Dutcher et al., 2015; contributing to CO2 sorption. Thus, it is projected that the
Chen C. et al., 2014; Gargiulo et al., 2014; Olajire, 2017). In a recent theoretic value for the maximum amine efficiency would be
book chapter (Wang and Song, 2019), we summarized the recent 0.5 (the blue dot line in the inset of Figure 7A). Clearly, most
advances of solid PEI-based sorbents for CO2 capture focusing on the PEI-based sorbents are still not able to achieve this theoretic
development of sorbent materials, the mechanism and kinetics in value, although there are a few reports showing their amine
CO2 sorption, the regeneration and deactivation, and the current and efficiency close to 0.5. Only one article reported the amine
future CO2 capture approaches. efficiency over 0.5, which was attributed to the contribution of

efficiency with high capacity, or whether there is a limit in the

amine efficiency in order to maintain the best CO2 sorption
capacity and kinetics.
With the aid of modern and advanced characterization
techniques, the CO2 sorption/deactivation mechanism over
PEI-based sorbents has been fundamentally better understood.
Zhang et al. studied CO2 sorption behavior with small angle
neutron scattering (SANS) technique and identified that the
swelling of PEI with CO2 sorption and temperature increase
played an important role in CO2 sorption process (Zhang et al.,
2019). Using solid-state nuclear magnetic resonance (SSNMR),
Mafra et al. (Mafra et al., 2017) found three chemisorbed CO2
species involving hydrogen bonds with either surface silanols or
amines. Chen et al. (2018) confirmed the formation of
bicarbonate in the presence of water. During CO2 sorption,
both carbamate and carbamic acid are formed (Foo et al.,
2017; Shimon et al., 2018), but only carbamic acid desorbs
while carbamate persists (Shimon et al., 2018). The formation
of CO and −CH N- species is a main reason for the air
degradation of amine sorbents (Ahmadalinezhad and Sayari,
2014). To improve the regeneration and long-term stability of
PEI-based sorbents, a two-step synthesis strategy involving
support modification followed by PEI loading has been
proposed and studied (Choi et al., 2016; Jeon et al., 2018; Min
et al., 2018a; Min et al., 2018b; Xu et al., 2018; Kim et al., 2019;
Wang et al., 2020), which have been summarized and elaborated
in our recent book chapter (Wang and Song, 2019).
Additionally, there has been important progress in the
development of adsorption processes for CO2 capture. A large
number of different cyclic regeneration processes using
temperature, pressure, vacuum, steam or moisture, or
combinations thereof have been studied. Recently, Inventys
Inc. (now is Svante Inc.) reported the VeloxoTherm process™
using a rotary unit packed with structured honeycomb adsorbent
FIGURE 7 | CO2 capacity reported in the literature with different support for both CO2 adsorption and desorption, which can complete a
at different PEI loading and temperature for CO2 capture from (A) pure CO2
and (B) from simulated air with about 400 ppm CO2 along with the insets
full cycle in about 60 s (Greeson, 2016). The comprehensively
showing the amine efficiency (A.E., mol-CO2/mol-N). All data are from review of the development of these processes can be found in the
the reported values (Wang and Song, 2019). literature (Grande and Rodrigues, 2008; Webley, 2014).
It should be pointed out that with the advance of the
technologies, some novel structured CO2 adsorbents have
CO2 physisorption on the porous support (Gaikwad et al., 2019). emerged, such as thin film nanocomposites (Shah and Imae,
As for the air capture (Figure 7B), most work was studied over 2016; Yong, 2016; Niranjana et al., 2019) and adsorbent-coated
the sorbents with PEI loading of 50 wt.% at room temperature. monoliths made of zeolites, MOFs, or carbons (Öhrman et al.,
Unlike CO2 capture from pure CO2, increasing temperature 2004; Ramos-Fernandez et al., 2011; Akhtar et al., 2014; Lee et al.,
results in the decrease of CO2 uptake, making it suitable for 2015). Monolithic contactors have substantial advantages like
air capture operation. Compared to those amine efficiency for uniform flow, high gas throughput, low pressure drop, and less
pure CO2, the amine efficiency for air capture is much lower, in attrition in comparison with conventional packed-bed reactors
between 0.05 and 0.15. It reflects that CO2 capture directly from (Rezaei and Webley, 2009; Rezaei and Webley, 2010). Both the
the air is more challenging than that from the concentrated CO2 diameter of the parallel channels and the density per cross-
sources. sectional area of monoliths are controllable. Most recently,
Figure 7 displays an indication of the current development three-dimensional (3D) printing or additive manufacturing
status of the PEI-based solid sorbents. Considering the low amine technique has gained worldwide attention and has been
efficiency compared to the theoretic value, especially for the air applied for fabrication of 3D-printed monoliths including
capture, we believe there is still a possibility to further enhance zeolites (e.g., 5A and 13X) and MOFs (MOF-74-Ni and
CO2 capture from both the concentrated sources and the air. UTSA-16-Co (Thakkar et al., 2016; Thakkar et al., 2017a;
Thus, further investigations are required to determine at what Thakkar et al., 2017b; Thakkar et al., 2018; Nguyen et al.,
level of PEI dispersion could be best for maximizing the amine 2019; Regufe et al., 2019; Thompson et al., 2019). Compared

to those prepared by conventional method, the 3D-printed their pore structure, thus receiving much attention (Alaslai et al.,
adsorbent materials exhibited comparable CO2 capacity, fast 2016; Yong et al., 2016; Gemeda et al., 2017). Siagian et al.
adsorption rate, and relative stability and regenerability. compared various polymeric membranes in terms of CO2/N2
Although 3D-printing shows flexibility in material design and selectivity vs. the permeability (Siagian et al., 2019). The
requires less steps and resources, extensive study on fabricating conventional polymers are not able to reach the desired
the adsorbent materials at large scale for carbon capture is performance for CO2 separation. The performance of TR
needed. membranes is close to the Robeson’s upper bond, while some
of PIM membranes show the performance above the Robeson’s
Membrane upper value, suggesting PIM membranes are more promising
Compared to other separation methods, membrane separation is than TR membranes for CO2 removal. However, more tests are
generally more energy efficient and environmentally benign, thus needed for these new membranes to be practical for CO2 capture
has been much studied for CO2 removal from flue gases (Merkel in industries.
et al., 2010; Japip et al., 2014). In membrane separation, the Hybrid membrane, or mixed matrix membrane (MMM),
driving force is the pressure and/or concentration difference. The which normally consists of an inorganic component such as
higher the pressure difference, the better the membrane zeolites, carbon nanotubes, silicates, alumina, or MOFs
separation. Therefore, it is more applicable to pre-combustion incorporated into the polymer matrix in the nanoparticles
capture processes, while it is quite challenging for post- form (Vinoba et al., 2017; Ahmad et al., 2018; Sarfraz and Ba-
combustion capture due mainly to the low CO2 partial Shammakh, 2018; Dilshad et al., 2019; Julian et al., 2019), is
pressure and/or concentration in the post-combustion flue becoming a new trend to improve polymeric membranes’
gases. Furthermore, unlike other methods, membrane properties, as it could possess both advantages of inorganic
separation involves multistage operation and streams recycling, and organic materials. Incorporating inorganic particles
which makes this method more complicated and complex. improves both the mechanical and thermal properties, making
Based on the properties of the fabrication materials, there are the polymeric membranes more stable. Thus, it provides a
three types of membranes in general (Powell and Qiao, 2006; Low solution to go beyond the restraint of polymeric membranes
et al., 2013): inorganic (or ceramic), organic (or polymeric), and and the inherent drawbacks of inorganic membranes in cost and
hybrid membranes. Those made up of zeolites, oxides (e.g., production (Ramasubramanian et al., 2012; Tanh Jeazet et al.,
Al2O3, TiO2, and ZrO2), ceramics, carbons, and MOFs are 2012; Bae and Long, 2013). MMM membranes show the potential
typical inorganic membranes (Al-Mamoori et al., 2017). to exceed the Robeson’s upper value and are comparable to the
Inorganic membranes are capable of high temperature PIM membranes. The main drawback for MMM membranes is
operation with good mechanical stability, but high fabrication that inorganic particles could be poorly dispersed, even
cost limits their scale-up (Al-Mamoori et al., 2017). Compared to aggregated within the polymer matrix, leading to membrane
inorganic membranes, polymeric membranes have several defects, deteriorating its overall performance (Zhang Y. et al.,
advantages including ease of synthesis, low production cost, 2013; Siagian et al., 2019). In addition, they are under early
good mechanical stability, and excellent separation development along with costly and complex fabrication processes
performance (Songolzadeh et al., 2014). Thus, more and more (Ramasubramanian and Ho, 2011).
polymeric membranes are practically replacing inorganic A new type of MMM membranes called facilitated transport
membranes in large-scale industrial gas separation processes hybrid membranes (FTHMs) or fixed carrier membranes (FCMs)
(Bernardo et al., 2009), and gradually dominating most has been proposed and studied (Wu et al., 2014). By
commercial membranes (Siagian et al., 2019). However, their incorporating the polymeric matrix with functional groups, it
thermal stability is relatively low, which curbs their application in exhibits fairly high CO2 permeability, CO2 selectivity, and
post-combustion CO2 capture. Flue gases normally have to be material stability (Wang S. et al., 2016), thus is promising as
cooled down first for membrane process (Du et al., 2011; Favre, next-generation membrane for CO2 separation. For example, at
2011). The separation performance of polymeric membrane 107°C and 15 bar, the CO2 permeability and the CO2/N2
materials can be further improved by incorporating or selectivity of the FCM containing amino-functionalized multi-
blending organic or inorganic compounds (Du et al., 2011; wall carbon nanotubes was 975 Barrer and 384, respectively
Dai et al., 2019). (Ansaloni et al., 2015). The CO2 permeance of 5693 GPU and
Recently, new types of polymeric membranes have been CO2/N2 selectivity of 268 were reported over the FCM
developed, for example, thermally rearranged (TR) and incorporated with nanosized hydrotalcite in
intrinsic microporosity polymeric (PIM) membranes. TR PEI–epichlorohydrin copolymer (PEIE) at around 25°C and
membranes exhibit improved thermal stability through 1.1 bar (Liao et al., 2014). Similar to other MMM membranes,
structural rearrangement and molecular transformation during one of the biggest challenges for industrial application of FCMs is
the heat treatment, which can generate interconnected to prepare the membranes without defects and the use of
microcavities with narrow size distribution, decreasing the nanosized carriers without agglomeration.
mechanical strength of TR membranes (Jo et al., 2015; Liu Q. Besides the membrane materials, the configuration of
et al., 2016; Scholes, 2016). PIM membranes are promising for membrane modules is also crucial. There are four main types
CO2 capture as they exhibit high CO2 permeability and of modular configurations mostly adopted: tubular, plate-and-
selectivity, surpassing the Robeson’s upper bond due largely to frame (Martín, 2016; Berk, 2018), spiral wound (Qi and Henson,

1998; Chen X. et al., 2015; Liu C. et al., 2016), and hollow fiber As above-pointed out, the high energy penalty for CO2 capture
(Yoshimune and Haraya, 2013; Chen X. et al., 2015; Esposito process is mainly caused by the low concentration or partial
et al., 2015; Liu C. et al., 2016). Compared to other types of pressure of CO2 in a flue gas, which results in high cost for CCS, as
modules, hollow-fiber membranes exhibit better popularity and the capture step accounts for about 70–80% of the overall CCS
more compact because of its optimum geometry and high cost (Figueroa et al., 2008). As shown in Table 2, the typical CO2
surface-to-volume ratio (Koros, 2004; Al-Mamoori et al., 2017; concentration in flue gases is about 3–14%. The current prevail
Wang Y. et al., 2017). Furthermore, highly porous polymeric economic analysis estimates a cost of $70–100/tonne-CO2 for
substructures supporting a thin selective layer of hollow fiber carbon capture from flue gas (Vitillo et al., 2017). With only
membranes show the potential in advancing the development of 400 ppm CO2 in air, a DACC process requires a cost between
membranes (Chen H. et al., 2014). $300 and $1,500 per tonne of CO2 captured (National Academies
of Sciences, Engineering, and Medicine, 2019). One viable
strategy is to increase the partial pressure or concentration of
FUTURE CONSIDERATION OF CARBON CO2 in flue gas. For example, through exhaust gas recycling, in
CAPTURE TECHNOLOGIES which flue gas from natural gas boiler (containing ∼4% CO2) is
recycled and used in place of air for the fuel combustion, CO2
Combination of Flue Gas Recycling and concentration in the flue gas can be enriched up to ∼8%, making
Hybrid Capture CO2 capture less thermodynamically challenging (Vaccarelli
The current development of CO2 capture processes has largely et al., 2014). However, considering the significant capital
centered on a single separation technology. Although numerous investment in exhaust gas recycling with respect to the
optimizations in materials and processes have been pursued, combustion unit, the balance between exhaust gas recycling
implementing a single separation process (e.g., aqueous amine- and carbon capture energy penalty has to be carefully and
based chemical absorption) is either energy intensive or costly. thoroughly examined and optimized (Vaccarelli et al., 2014).
Only few studies have looked at integrating two or more Membranes can also be utilized to concentrate CO2 from flue
technologies (i.e., absorption, adsorption, membrane, and gas for recycling. Merkel et al. obtained up to 20% increase in CO2
cryogenic) into a hybrid process for CO2 capture (Freeman concentration and up to 40% reduction in the minimum energy
et al., 2014). The integration of different separation required for CO2 capture (Merkel et al., 2013). A set of
technologies could avoid their individual disadvantages, thus membranes in series or parallel may be used for selective CO2
may be superior to the standalone process (Scholz et al., 2013). recycling, offering increased driving force for CO2 separation. It
Recently, Song et al. reviewed the hybrid CO2 capture could be more efficient if coupled with other capture technologies
technologies and explored possible combinations (Song et al., (e.g., absorption, adsorption, and cryogenics), especially with
2018), including absorption-, adsorption-, membrane-, and those hybrid systems.
cryogenic-based hybrid processes with different options. Although it could increase capital and maintenance costs,
Nakhjiri and Heydarinasab compared the performance of the recycling flue gas or pre-concentrating CO2 with membranes can
hybrid membrane absorption process using ethylenediamine simplify the CO2 capture process. By combining the advantages of
(EDA), 2-(1-piperazinyl)-ethylamine (PZEA), and potassium hybrid CO2 capture systems, we believe that the benefits in the
sarcosinate (PS) absorbents (Nakhjiri and Heydarinasab, subsequent CO2 capture step could be substantial, which may
2019). They found that the CO2 separation efficiency decreases ultimately make this approach more energy efficient and cost
as PZEA > PS > EDA. Atlaskin et al. (Atlaskin et al., 2020) studied effective. Although currently the experimental data are not
a hybrid membrane-assisted gas absorption (MAGA) process for enough, the primary results have convinced us that the
CO2 and H2S removal. The efficiency for CO2/H2S separation was proposed concept would be plausible as future CCS direction,
significantly increased by mixing imidazolium ionic liquid (ca. 5 v especially to overcome the technical bottlenecks encountered
%) into the methyldiethanolamine (MDEA) solution. Over the when using single carbon capture technology.
hybrid membrane absorption system using 2-methylpiperazine
(2MPZ)-promoted potassium carbonate for CO2 separation, One-Step Integrated CO2 Capture and
increasing 2MPZ concentration, absorbent flow rate, porosity Conversion
to tortuosity ratio, and membrane fibers can enhance the CO2 Another encouraging strategy is integrating the CO2 capture and
removal percentage up to over 98% (Izaddoust and Keshavarz, conversion in one stage. In nature, organisms or organelles
2017; Mesbah et al., 2019). Scholes et al. recently reported the indeed systematically utilize and store CO2 directly. However,
pilot plant trials with hollow fiber membrane-MEA (MEA, 30 wt compared to chemical-based approaches, they are much limited
%) contactor for post-combustion CO2 capture, showing the by the long time and large contact area requirements (Table 3).
energy duty less than 4.2 GJ/ton of CO2 captured (Scholes When CO2 capture is integrated directly with subsequent in situ
et al., 2020). Through the comparison to the standalone CO2 utilization/conversion to value-added products in one step,
methods, they found that the hybrid processes are superior in the concept of which is depicted in Figure 8, the process could
terms of CO2 recovery, energy penalty, and installation eliminate the needs of the steps for CO2 desorption, compression,
investment, thus are promising as future carbon capture transportation, and storage, eradicating the energy penalty
technology (Song et al., 2018). associated with these steps. It is particularly useful to the

FIGURE 8 | Concept of one step direct integration of CO2 capture and in situ CO2 conversion.
chemical absorption-based CO2 capture technologies, where the solutions for CO2 capture followed by in situ hydrogenation using
significant energy penalty occurs at the desorption step. coexisted homogeneous metal complex catalysts to formate salts
Furthermore, the production of value-added chemicals and and methanol (Kar et al., 2019). The whole process is regenerable
fuels could generate revenues to compensate the cost for for multiple cycles. Consequently, they suggested that the amine-
carbon capture, which helps reducing the economic barrier for assisted CO2 capture and conversion to methanol process is very
the commercial deployment of the CO2 capture technologies. encouraging. Stuardi et al. also suggested the integration of CO2
This is also a pathway to functionalizing metal–organic capture and utilization as a priority research direction (Marocco
frameworks, electrocatalysts, photocatalysts, and more—for Stuardi et al., 2019).
their potential applications in CO2 capture and conversion. Besides the liquid amine processes, the solid adsorbent
Recent years, more reports about the one-step integration of catalyst-based CO2 capture-conversion processes using dual
CO2 capture and conversion are coming out. Gassner and Leitner function materials (DFMs) consisting of the methanation
first reported the attempt to integrate catalytic CO2 conversion to catalyst (e.g., Ru and Ni) and CO2 adsorbent (e.g., CaO,
capture via CO2 hydrogenation to formate in the presence of Na2O, and MgO) on a support have also been studied at mild
aqueous amine solutions (Gassner and Leitner, 1993). He et al. conditions (200–350°C and 1 atm) (Duyar et al., 2015; Duyar
explored a combined system containing a superbase, a poly et al., 2016; Miguel et al., 2017; Wang S. et al., 2017; Wang et al.,
(ethylene glycol) (PEG), ionic liquid and amino acid for in 2018; Arellano-Treviño et al., 2019; Zhou et al., 2020).Those
situ CO2 capture-conversion to carbonates, urea, and formate DFMs exhibit stable performance in CO2 capture and conversion
salts (Yang et al., 2011a; Yang et al., 2011b; Liu et al., 2012). Kim to synthetic CH4 for over 50 cycles. No loss in CO2 capture
et al. experimentally demonstrated a process directly integrating capacity and Ru dispersion was observed (Wang et al., 2018).
CO2 utilization into CO2 capture, allowing for the full conversion Over the 2D-layered Ni–MgO–Al2O3 nanosheets, continuous
of the CO2 captured into syngas in a single reactor using and nearly 100% capture of CO2 during prolonged cycling
limestone for CO2 capture and a non-precious metal catalyst tests was achieved at temperatures below 250°C (Zhou et al.,
for CO2 conversion with CH4 (Kim et al., 2018). Liu et al. 2020). Its hydrogen efficiency reached 60% for CO2 conversion to
developed a novel hybrid MgAl(LDO)/TiO2 adsorbent/ CH4, making the process attractive for large CO2 emission
photocatalyst for the integrated CO2 capture plus sources.
photocatalytic conversion directly to C1 products at Patterson et al. proposed an approach to recycle atmospheric
100–200°C (Liu et al., 2015). The regeneration of the CO2 into liquid fuels on a large-scale marine-based artificial
developed material can be easily achieved with low-grade island, using renewable energy (solar or wind) to power the
waste heat and/or solar energy (Liu et al., 2015). Kar et al. production of hydrogen and CO2 extraction from seawater,
systematically reviewed the current progress in the integrated followed by catalytic conversion to liquid methanol fuel
capture-conversion process using aqueous amine and hydroxide (Patterson et al., 2019). The major advantage of the proposed

approach is the utilization of sea as the CO2 absorber, in which it capture technologies with improved energy efficiency and cost-
is always in equilibrium with the atmosphere, along with the effectiveness. In this perspective, we believe the two plausible
usage of renewable energy, generating negative CO2 emission approaches, that is, the combination of flue gas recycling and
through the process. hybrid capture system, and one-step integration of CO2 capture
These efforts in the integration of CO2 capture and conversion and conversion, are promising for future research, as they could
in one step have demonstrated their promise, although mainly C1 offer significant improvement in energy efficiency and cost-
products are generated. Through the research entailing effectiveness, by simplifying the capture process in the former
experimental results coupled with theory to improve and eliminating the desorption, compression, transportation, and
fundamental understanding, and the design of innovative storage steps in the latter, respectively. However, more research
polyfunctional and multi-structured materials for the one-step and development such as materials development, synergistic
integrated CO2 capture and conversion, the production of liquid assessment, process design, process optimization, and scale-up
hydrocarbon fuels, chemicals, polymers, carbon materials (e.g., are required. Their environmental impacts and the life-cycle
nanotubes and nanofibers) directly from flue gas or atmospheric analysis should also be considered. Nonetheless, the proposed
CO2 can be envisaged in future. It will also lead to developing and emerging approaches appear to be promising with better
carbon capture technologies with smaller size, greener process, commercial potential in the future, and offer a viable solution to
and better energy efficiency. If implemented, it could significantly the technical bottlenecks of current carbon capture technologies,
change the way in CO2 capture, compress, transport, conversion, and to the global dilemma in meeting more energy demand while
and/or storage, thus increasing opportunities for CO2 reducing environmental impact.
valorization, and offer a feasible solution to the current global
environmental problems associated with energy use.
AUTHOR CONTRIBUTIONS
CONCLUDING REMARKS All authors listed have made a substantial, direct, and intellectual
contribution to the work and approved it for publication.
Through the past few decades of research and development, there
have been significant progresses in CO2 capture technologies, but
still far from economically attractive commercialization. It ACKNOWLEDGMENTS
requires a comprehensive investigation on the characteristics
and relationships of the materials and process performance, The financial support from the Pennsylvania State University and
which is crucial to the development of next-generation carbon EMS Energy Institute Seed Grant is appreciatively acknowledged.
Al-Mamoori, A., Krishnamurthy, A., Rownaghi, A. A., and Rezaei, F. (2017).

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acsami.9b08496 absence of any commercial or financial relationships that could be construed as a
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Carbon Capture From Flue Gas and The Atmosphere: A Perspective

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published: 15 December 2020

Carbon Capture From Flue Gas and

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FIGURE 1 | Atmospheric CO2 concentration during 1950–2019 (data sources: http://climate.nasa.gov/vital-signs/carbon-dioxide/).

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FIGURE 2 | Schematic diagram of the existing CO2 capture pathways.

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extraction, making this pathway more energy intensive and

• H2-rich gas-induced temperature and efﬁciency issues

• Retroﬁt unattractive due to Signiﬁcant plant changes

• Costly and energy intensive air separation step

gases with a high concentration of CO2, which could be captured

and directly used or transported for storage after some

• Immature, currently under development

• Immature, currently under development

puriﬁcation. Similar to the oxy-combustion and CLC

• High capital and operating costs

needed for those processes.

Figure 3 illustrates various CO2 capture technologies including

industry for the past few decades, while Table 3 brieﬂy

available, especially in the petroleum and chemical industries.

Based on the nature of the interaction between the absorbent and

CO2, it separates as chemical absorption (mainly applied for CO2

(mainly used for CO2 capture from pre-combustion ﬂue gas).

diethanolamine (DEA)) and liquid ammonia are typical

solvents for chemical absorption. MEA solution has become

✓Very high CO2 concentration

the benchmark amine for CO2 capture from power plants

biodegradable. However, it suffers from toxicity and solvent loss

cost-effective carbon capture absorption technology. So far, a

large number of solvents, including single amines, amine blends,

and amino acids, have been evaluated individually for their

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Flue gas source CO2 conc. (%) P (atm) CO2

Gas turbine 3–4 1 0.03–0.04

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Wang and Song

Technology Mechanisms Pros Cons

A Perspective on CO2 Capture

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efﬁciency with high capacity, or whether there is a limit in the

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Al-Mamoori, A., Krishnamurthy, A., Rownaghi, A. A., and Rezaei, F. (2017).

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