1. Introduction

Elevation of carbon dioxide (CO₂) gas concentration in the atmosphere is the major factor contributing to global warming. In recent years, CO₂ emissions reached a record level, primarily as a result of the burning of fossil fuels [1]. Carbon capture and storage/sequestration (CCS) is crucial in order to prevent the atmosphere's CO₂ concentration from rising. Pre-combustion, post-combustion, oxy-fuel combustion, and direct air capture are the main methods used to capture CO₂. Out of these methods, post-combustion capture of CO₂ is operationally simple and useful in many industries and power sectors, such as coal-fired power plants [2]. An efficient technique for post-combustion CO₂ capture is the adsorption of gas onto the surface of solid sorbent. Polymers and polymer-based materials are discovered to be particularly promising among several forms of solid sorbents. An efficient and very sustainable method of CO₂ capture is the use of non-toxic, affordable, and widely available polysaccharide-based biopolymers. Porous materials used in CO₂ capture are usually prepared by carbonization and physical or chemical activation of the chosen biopolymers [3].

Since CCS is an important and cutting-edge field of study, a huge number of research articles have been published in the past two decades. Worldwide, there has been a tremendous increase in the development of novel porous materials [3-6]. In this scenario, a comprehensive report is needed to inform the readers of the most recent advancements on the development of new biopolymer-derived materials and their applications in CCS. We have compiled the synthetic methods, post-synthetic changes, and CO₂ capture capacities of various biopolymer-based materials published in the recent five years (2018-2022). We also briefly touched on the factors that affect the selectivity and capacity of CO₂ capture.

2. Types of Biopolymers and Mechanism of Adsorption of CO₂

In the capture and storage of CO₂, both natural and synthetic polymers are widely used. Polysaccharides that have proven to be highly useful in CO₂ capture and storage applications include cellulose, chitosan, lignin, and cyclodextrins. Porous materials derived from polysaccharides capture CO₂ gas by adsorption on the surface. Physical adsorption, also known as physisorption, and chemical adsorption, known as chemisorption, are the two types of adsorption processes. Through non-covalent interactions (Coulombic, Van der Waals, etc.), physisorption takes place on the adsorbent's surface. In this instance, desorption of the gas molecules is a low-energy process. Adsorbents can be reused repeatedly, which is a key benefit of physisorption. On the other hand, reduced selectivity and a low adsorption capacity of the adsorbent at high temperatures are disadvantages. In chemisorptions, gas molecules and the surface of the adsorbent create covalent bonds. On the surface of common adsorbents, there are basic functional groups like amine. Basic functional groups react with acidic CO₂ molecules to produce salts. High adsorption capacity and superior selectivity of the adsorbents are chemisorption's main benefits. This process often has energy-intensive sorbent regeneration as a downside [7].

Isosteric heat of adsorption (Q_st) value, calculated by fitting adsorption isotherms by using the Clausius–Clapeyron equation, indicates strength of interaction between adsorbents and CO₂ molecules. A low Q_st value points to a predominance of physisorption, whereas a high Q_st value points to a strong interaction between the surface of the material and the gas molecules, resulting to a predominance of chemisorption. Effective separation requires good adsorbents to preferentially absorb CO₂ over all other gases. CO₂/N₂ selectivity is thus a crucial indicator for CO₂ capture by adsorbents. Henry's law and the ideal adsorption solution theory (IAST) are used to compute the CO₂/N₂ selectivity. Additionally significant elements that influence adsorption efficacy are the adsorbents' porosity and surface area. The Brunauer-Emmett-Teller (BET) theory is commonly used to assess the surface areas of the adsorbents [8].

3. Polysaccharide-Based Biopolymers for CO₂ Capture

Over years biopolymers are utilized for designing biomaterials for various applications such as packaging materials in the food industry, fuel cells, drug delivery, membrane and medical implants organ preparation, tissue engineering and many more [9–14]. Polysaccharides are cheap and abundant carbohydrate-based biopolymers which has multiple applications [3,15–22]. In studies of CO₂ capture and storage, cellulose, chitosan, lignin, and cyclodextrins are some of the most often used polysaccharides due to their wide availability, simplicity of processing, tolerance to structural modifications, and solubility [3]. The following is a summary of applications of these four key types of biopolymers in CCS that have been documented over the last five years.

3.1. Cellulose-Based Materials for CO₂ Capture

Cellulose is a linear polysaccharide consisting of repeated D-glucose units with the formula of (C₆H₁₀O₅)_n. In a recent study, bottom-up ecosystem simulation is coupled with models of cellulosic biofuel production, carbon capture and storage to track ecosystem and supply chain carbon flows for current and future biofuel systems. This approach could have climate mitigation and stabilization potential [20]. Different types of polysaccharides for CO₂ capture have been reported by Qaroush et al, describing the reversible reaction between cellulose and CO₂, their subsequent dissolution, regeneration and CO₂ capturing using functionalised cellulosic materials [3]. One interesting approach for CO₂ capture is converting cellulose to sustainable porous carbon materials [21]. Porous carbonaceous materials are usually prepared by carbonization and activation [21]. Carbonization process can be of two types, (i) pyrolytic approach which involves heating the sample at elevated temperatures of 400–1000 °C in an inert atmosphere (e.g., N₂, Ar). Several steps included in pyrolytic approach like dehydration, condensation and isomerization, which ultimately eliminates most of the hydrogen and oxygen atoms to form H₂O, H₂, CH₄, and CO gases. Other approach (ii) Hydrothermal carbonization (HTC) is usually performed at moderate temperatures (<300 °C) and advantageous due to reduced energy consumption, sample does not need to be dry and gives carbon-rich hydrochars in high yields. Thus in recent times, the HTC method is considered an energy-saving and environmentally friendly approach for carbonization [21]. Two activation methods are being reported which produce porous carbons with large differences in porosity. In general, physical activation processes create porous carbons with moderate surface areas (1000 m²/g) and narrow micropores that can be beneficial for, e.g., CO₂/N₂ and CO₂/CH₄ separation [21]. In contrast, chemical activation significantly increases the surface area (up to >3000 m²/g) and pore volume of the porous carbons which can be useful for gas storage [21]. Here CO₂ adsorption capacity of some cellulose-derived materials derived by the carbonization process are discussed. A series of porous carbons derived from commercial cellulose fibres in three steps has been reported by Heo et al. They described that steam molecules played a key role in the pore-opening process and increase in the surface area of the porous carbon materials formed. The cellulose fibres were carbonized under N₂ atmosphere followed by physical activation with steam under gauge pressure. Ultramicropores (pore size < 0.8 nm) resulted by physical activation process significantly contributed to the increase in surface areas from 452 to 540 m²/g for pre-activated samples to 599–1018 m²/g for steam-activated samples causing CO₂-over-N₂ adsorption selectivity and increase in CO₂ adsorption capacity by physical adsorption method [22]. In a following study, Zhuo et al. reported a hierarchically porous carbons prepared by carbonization/activation of cellulose aerogels under CO₂ and N₂ atmosphere with improved surface area and volume for CO₂ adsorption. They showed that steam activation is an efficient process to prepare cellulose-based porous carbons with high CO₂ adsorption capacities by physisorption [23].

Chemically activated carbonaceous materials have much higher surface areas thus resulting in much higher CO₂ adsorption capacities. Chemical activation of cellulose by KOH was reported by Sevilla et al. to design microporous carbon materials with a very high surface area of 2370 m²/g and CO₂ adsorption capacity of 5.8 mmol g⁻¹ at 1 bar and 273 K at a high adsorption rate and excellent adsorption recyclability by physisorption mechanism. The material was prepared by hydrothermal carbonization of potato starch, cellulose and eucalyptus sawdust followed by chemical activation using potassium hydroxide [24]. In another study by Xu et al., algae-extracted nanofibrous chemically modified cellulose carbonized under N₂ and CO₂ atmosphere and activated in CO₂ was reported to show significantly higher surface areas (832–1241 m²/g) and higher volumes of ultramicropores (0.24–0.29 cm³/g) for CO₂ physisorption [25]. In recent times, cellulose aerogels have also displayed promising applications in carbon storage. A review has been reported by Ho et al. depicting chemical modification of nanocellulose aerogels leading to a large surface area which improved selectivity towards CO₂ chemisorption [26]. Kamran et al. utilized hydrothermal carbonization method and chemical activation with acetic acid as an additive, to develop highly porous carbons. These cellulose-based materials displayed high specific surface area (SSA) (1260–3019 m² g⁻¹), microporosity in the range of 0.21–1.13 cm³ g⁻¹ with CO₂ adsorption uptake of 6.75 mmol g⁻¹ and 3.96 mmol g⁻¹ at 273 K and 298 K at 1 bar, respectively, and CO₂ selectivity by physisorption mechanism. The carbonaceous material having micropores between 0.68 nm and 1 nm exhibited high CO₂ adsorption potential [27].

However non-carbonized cellulose-derived materials have also been reported for efficient CO₂ adsorption capacities. In this regard, Wang et al. and Sun et al. have reported that cross-linking of nanocellulose enhances the surface area and CO₂ adsorption [28,29]. Amino-functionalization of nanocellulose aerogels although reduced the surface area but still displayed chemisorption of CO₂ with a capacity of more than 2 mmol g⁻¹ [26]. In some other reports, cellulose hybrids were designed without any carbonization with inorganic fillers such as silica, zeolite and metal–organic frameworks which improved the surface area and physisorption of CO₂ [26]. Sepahvand et al. have designed nano filters by combining cellulose nanofibers (CNF) and chitosan (CS) at varied loading compositions. Increasing the concentration of modified CNFs increases the adsorption rate of CO₂ and the highest adsorption of CO₂ was showed by 2% modified CNF [30]. In a recent study, epoxy-functionalized polyethyleneimine modified epichlorohydrin-cross-linked cellulose aerogel with rich porous structure and specific surface area in the range of 97.5–149.5 m²/g has been reported by Chen et al. Good adsorption performance by chemisorption mechanism, with a maximum CO₂ adsorption capacity of 6.45 mmol g⁻¹ was displayed by the epoxy functionalized cellulose aerogels[31]. Material type and composition, BET surface area (m² g⁻¹), pore size (nm)/total pore volume (cm³ g⁻¹), mechanism of adsorption, CO₂ capture capacity (mmol g⁻¹) and special features of cellulose-based materials have been tabulated in Table 1.

Table 1. Summary of material type and composition, BET surface area (m² g⁻¹), pore size (nm)/total pore volume (cm³ g⁻¹), CO₂ capture capacity (mmol g⁻¹) and special features of cellulose-based materials.

One important class of nanocellulose-based materials and their subsequent application involves membrane separation of CO₂. In this regard, Ansaloni et al. reported micro fibrillated cellulose/Lupamin membrane which showed very good CO₂ permeability. However the selectivity of CO₂/N₂ and CO₂/CH₄ (in the order of 500 and 350, respectively, for pure micro cellulose) was compromised thus decreasing the overall membrane performance [32]. Venturi et al. later did a systematic study of CO₂ permeability by nanocellulose-based membranes under the influence of doping. They designed films by blending the commercial Polyvinylamine solution Lupamin^® 9095 (BASF) with Nano Fibrillated Cellulose (NFC). It was reported that, increasing water vapour and a higher presence of Lupamin in the film improved CO₂ gas permeability as well as selectivity. NFC content of 70 wt% Lupamin showed a selectivity of 135 for the separation of CO₂/CH₄ and 218 for CO₂/N₂ while the maximum permeability in the order of 187 Barrer was reached at 80% RH [33]. In a follow up study by the same group, the addition of l-arginine to a matrix of carboxymethylated nano-fibrillated cellulose (CMC-NFC) resulted in a mobile carrier facilitated transport membrane for CO₂ separation. l-arginine (45 wt.% loading) greatly improved CO₂ permeability by 7-fold from 29 to 225 Barrer and selectivity with respect to N₂ from 55 to 187 compared to pure carboxymethyl nanocellulose matrix [34]. Pure and mixed matrix membranes (MMMs) with polyethylene glycol (PEG), Multi-walled carbon nanotubes (MWCNTs) and cellulose acetate (CA) has been reported by Hussain et al to capture carbon from natural gas. Membranes of pure CA, CA/PEG blend of different PEG concentrations (5%, 10%, 15%) and CA/PEG/MWCNTs blend of 10% PEG with different MWCNTs concentrations (5%, 10%, 15%) were designed. The CO₂/CH₄ selectivity is enhanced 8 times for pure membranes containing 10% PEG and 14 times for MMMs containing 10% MWCNTs and in mixed gas experiments, the CO₂/CH₄ selectivity is increased 13 times for 10% PEG and 18 times for MMMs with 10% MWCNT [35]. Composite membranes using non-stoichiometric ZIF-62 MOF glass and cellulose acetate (CA) are reported by Mubashir et al. The materials exhibited pore size (7.3 Å) and significant CO₂ adsorption on the unsaturated metal nodes [36]. In more recent studies, another class of mixed matrix membranes (MMMs) are reported by Rehman et al. by incorporating (1–5 wt%) Cu-MOF-GO composites as filler into cellulose acetate (CA) polymer matrix by adopting the solution casting method. They reported 1.79 mmol g⁻¹ and 7.98 wt% of CO₂ uptake at 15 bar [37]. Some other foam-like cellulose composites reported by Wang et al with microporous metal–organic frameworks (MOFs) in a mesoporous cellulose template shows high durability during the temperature swing cyclic CO₂ adsorption/desorption process and a high CO₂ adsorption capacity of 1.46 mmol g⁻¹ at 25 °C and atmospheric pressure [38].

3.2. Chitosan-Based Materials for CO₂ Capture

Natural biopolymer chitosan (CS) is a marine waste material which is inexpensive, abundantly available, renewable, environmentally friendly and biodegradable polysaccharide and is the second most abundant natural polysaccharide after cellulose [39]. CS may be used in CO₂ adsorption because of its ease of processability, low maintenance and energy necessity. CS chains have a large number of basic amine groups which facilitate adsorption of the acidic CO₂ molecule on the surface of the adsorbents [40,41]. However, pure chitosan suffers from low surface area resulting lower carbon dioxide adsorption. Henceforth, most of the studies reporting chitosan-derived sorbents aim to fabricate the surface properties of CS and maximize the CO₂ adsorption capacity [42]. Hierarchical porous nitrogen-containing activated carbons (N-ACs) were prepared with LiCl-ZnCl₂ molten salt as a template derived from cheap chitosan via simple one-step carbonization under Ar atmosphere. The obtained N-ACs with the highest specific surface area of 2025 m² g⁻¹ and a high nitrogen content of 5.1 wt% were obtained using a low molten salt/chitosan mass ratio (3/1) and moderate calcination temperature (1000 °C). Importantly, using these N-ACs as CO₂ solid-state adsorbents, the maximum CO₂ capture capacities could be up to 7.9/5.6 mmol g⁻¹ at 0 °C/25 °C under 1 bar pressure, respectively by physisorption mechanism. These CO₂ capture capacities of N-ACs were the highest compared to reported biomass-derived carbon materials, and these values were also comparable to most of porous carbon materials. The N-ACs also showed good selectivity for CO₂/N₂ separation and excellent recyclability [43]. Chagas et al. reported a green method for CO₂ capture by showing the effects of hydrothermal carbonization (HTC) on chitosan’s chemical properties and its potential. Chitosan’s surfaces and structural properties are modified after HTC which increases the CO₂ adsorption capacity by 4-fold compared to the non-HTC treated chitosan [44]. Acetic acid-mediated chitosan-based porous carbons were developed by Kamaran et al. following a combination of hydrothermal carbonization treatment and chemical activation with KOH and NaOH under a flowing stream of nitrogen. The CO₂ uptake was reported to be 8.36 mmol g⁻¹ for KOH samples and 7.38 mmol g⁻¹ for the NaOH sample. These synthesized carbon adsorbents also exhibited regenerability after four consecutive adsorption–desorption cycles and also high CO₂ selectivity over N₂ gas [45].

Azharul Islam et al. have reported a non-carbonized chitosan–bleaching earth clay composite (Chi–BE) as an efficient adsorbent for CO₂. They showed that temperature, adsorbent loading and CO₂ concentration exerted significantly positive effects on CO₂ adsorption by Chi–BE within the ranges and levels studied, whereas the interaction of adsorbent loading and CO₂ concentration only affected CO₂ adsorption. The optimum conditions were 38.13 °C, adsorbent loading of 0.72 g and CO₂ concentration of 25%, which produced the adsorption capacity of 7.84 mmol g⁻¹ using the desirability function and the composite can also be recycled [46]. Material type and composition, BET surface area (m² g⁻¹), pore size (nm)/total pore volume (cm³ g⁻¹), mechanism of adsorption, CO₂ capture capacity (mmol g⁻¹) and special features of chitosan-based materials have been tabulated in Table 2.

Table 2. Summary of material type and composition, BET surface area (m² g⁻¹), pore size (nm)/total pore volume (cm³ g⁻¹), mechanism of adsorption, CO₂ capture capacity (mmol g⁻¹) and special features of chitosan-based materials.

3.3. Lignin-Based Materials for CO₂ Capture

Lignin is a class of complex organic polymers found in plants particularly important in the formation of cell walls, especially in wood and bark. Chemically, lignins are polymers made by cross-linking phenolic precursors. The synthesis of multiscale carbonized carbon supraparticles (SPs) by soft-templating lignin nano- and microbeads bound with cellulose nanofibrils (CNFs) have been reported by Zhao et al. which were well suited for CO₂ capture (1.75 mmol g⁻¹), while displaying a relatively low pressure drop (~33 kPa·m⁻¹ calculated for a packed fixed-bed column). Moreover, the carbon SPs did not require doping with heteroatoms for effective CO₂ uptake and also showed regeneration after multiple adsorption/desorption cycles [47]. Non-carbonized lignin-based materials have been reported by Shao et al. and Liu et al. [48,49]. Lignin depolymerization was done selecting six aromatic units from lignin and O-rich hyper-cross-linked polymers (HCPs) was developed by one-pot Friedel–Crafts alkylation reaction for CO₂ capture. In a recent report, the resins were synthesized from lignin, 4-vinylbenzyl chloride, and divinylbenzene by free radical polymerization reaction followed by Friedel–Crafts reaction which displayed excellent CO₂ capture (1.96 mmol g⁻¹) at 273 K and 1 bar and reusability [49].

3.4. Cyclodextrin-Based Materials for CO₂ Capture

Cyclodextrins are glucopyranosides bound together in various ring sizes renowned for their structural, physical and chemical properties. Due to their unique ability to encapsulate other molecules, they are widely used in industrial applications [50]. The cyclodextrin (CD)/graphene composite aerogel synthesized by hydrothermal carbonized reaction at 80 °C for 18 h exhibits an adsorption capacity of CO₂ at 1.02 mmol g⁻¹ [51]. Cyclodextrin-based non-carbonized materials also reported to be efficient CO₂ adsorbent [52–54]. Two isostructural cyclodextrin-based CD-MOFs (CD-MOF-1 and CD-MOF-2) are demonstrated to have an inverse ability to selectively capture CO₂ from C₂H₂ by single-component adsorption isotherms and dynamic breakthrough experiments. These two MOFs exhibit excellent adsorption capacity and selectivity (118.7) for CO₂/C₂H₂ mixture at room temperature [52]. A new solid acid adsorbent for CO₂ capture derived from β-cyclodextrin has been obtained which shows a capacity of 39.87 cm³/g at 3.5 bar [53]. For thermal activation, a rapid temperature-assisted synthesis has been reported to improve the porous structure of the cyclodextrins for CO₂ adsorption [54]. Another category of cyclodextrin-based materials involves CO₂ adsorption by thermal activation under N₂ atmosphere [55,56].

4. Conclusions

In this review, we have provided an overview of the synthesis, CO₂ capture potential, and key factors influencing the CO₂-philicity of several natural polymer-derived materials that have been described in the literature over the last five years. Despite the relatively low CO₂ capture capabilities of biopolymers, microporous and nanoporous materials made from them showed good adsorption capability. Particularly, membranes made of nanocellulose were discovered to be prospective candidates for the large-scale capture and separation of CO₂ from flue gas. In the study for creating novel materials for post-combustion CO₂ capture and separation, biopolymers have played a significant role. Large-scale CO₂ capture requires solid adsorbents that have strong moisture resistance, large surface area (>1000 m²/g), abundant micropores, >2 mmol g⁻¹ CO₂ adsorption capacity, and >100 CO₂/N₂ selectivity. At the same time, the adsorbent's mass manufacture must be economical.

Using biopolymers to capture CO₂ has made significant progress thus far, but there are still many obstacles to overcome. Surface modification and processability are hampered by many biopolymers' low solubility in common solvents. As a result, creation of membranes, which are very helpful for large-scale CO₂ capture and separation, becomes problematic. Flue gas has a partial pressure of CO₂ as low as 3-15 kPa and a temperature between 80 and 90 °C. Therefore, it is necessary to increase the CO₂ capture capabilities of biopolymer-derived materials at high temperatures and low pressures.

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This entry is adapted from the peer-reviewed paper 10.3390/polysaccharides4020012