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Biological Metal-Organic Framework Materials for CO2 Capture Performance

Hao Wang , Xi Liu , Kongkong Zhao , Shuzhao Pei , Zhida Li , Hongjun Wu

Progress in Chemistry ›› 2026, Vol. 38 ›› Issue (5) : 941 -956.

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Progress in Chemistry ›› 2026, Vol. 38 ›› Issue (5) : 941-956 DOI: 10.7536/PC20250709
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Biological Metal-Organic Framework Materials for CO2 Capture Performance
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Abstract

Efficient capture and selective separation of CO2 is one of the important means to realize the “dual carbon” goal and mitigate climate change， and metal-organic frameworks （MOFs） show great potential in gas separation and storage due to their structural peculiarities. The potential of MOFs in the field of gas separation and storage is enormous. Among them， biological metal-organic framework （Bio-MOFs） are constructed by green synthesis pathway using natural biomolecules （e.g.， amino acids， nucleobases， peptides， etc.） as ligands， and they are both environmentally friendly and cost-effective， providing innovative solutions for CO2 capture. This paper will focus on the following： systematically summarizing the structural properties of the bio-ligands and their modulation of the framework pores and chemical properties； exploring the mechanism of direct synthesis and post-synthesis modification （e.g.， amine functionalization， ion exchange） and other strategies to enhance the performance of the materials； analyzing the adsorption behaviors of the Bio-MOFs of CO2 in complex media， elucidating the synergistic roles of molecular sieving， equilibrium sieving， and gating effects； and analyzing the CO2 adsorption behaviors of the Bio-MOFs in complex media， synergistic effect； and the challenges and future development direction of Bio-MOFs are also prospected.

Contents

1 Introduction

2 Overview of Bio-MOFs

2.1 Basic definition and characteristics of Bio-MOFs

2.2 Bio-MOFs constructed from bio-like molecules

2.3 Derived Bio-MOFs （biomolecule-MOF hybrid structures）

3 Application of CO2 adsorption of Bio-MOFs

3.1 Classification of CO2 adsorption behavior by bio-MOFs

3.2 CO2 adsorption by Bio-MOFs

3.3 Derived Bio-MOFs CO2 adsorption

4 Summary and prospects

Graphical abstract

Keywords

biological metal-organic framework（Bio-MOFs） / CO2 capture / porous materials / functionalized modifications / adsorption

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Hao Wang, Xi Liu, Kongkong Zhao, Shuzhao Pei, Zhida Li, Hongjun Wu. Biological Metal-Organic Framework Materials for CO2 Capture Performance. Progress in Chemistry, 2026, 38(5): 941-956 DOI:10.7536/PC20250709

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1 Introduction

The growing global population and accelerating industrialization are continuously increasing energy demand. According to the International Energy Agency (IEA),[1-2]: In 2022, global energy-related CO2 emissions reached 36.8 Gt, a 0.9% increase from 2021, hitting a record high. The rise in CO2 concentration has led to global warming and frequent extreme weather events, seriously threatening ecological and socio-economic security. Developing efficient and environmentally friendly Carbon Capture, Utilization, and Storage (CCUS) technologies is crucial for achieving the "dual carbon" goals and ensuring energy security.[3-4]. Within the CCUS system, CO2 capture (CCS) is the key link affecting overall costs.[5]Compared to traditional chemical absorption[6-7]and cryogenic distillation[8-9], gas separation technologies based on porous materials offer advantages such as low energy consumption, strong regenerability, and environmental friendliness.[10].
Metal-organic framework (MOF) materials formed by the self-assembly of inorganic metal nodes or clusters with organic linkers via coordination bonds[11-13], possess abundant and easily tunable pore structures[14-15], controllable internal pore environments[16], ultra-high specific surface areas[3,12], low density, and functionalized framework structures[17], as well as diverse varieties[18-19]. The flexibility of MOF materials enables the introduction of specific functional adsorption sites, such as Lewis basic/acidic sites, uncoordinated N atoms, or coordinatively unsaturated metal centers (open metal sites), thereby achieving controlled adsorption of guest molecules[20]. Furthermore, by selecting hard acid metal ions (Zr/Hf clusters), MOFs can also exhibit high thermal and chemical stability. Leveraging these unique physicochemical properties, MOF materials demonstrate immense application potential in fields such as gas separation, catalysis, and biomedicine[21].
However, traditional MOFs mostly use non-renewable aromatic carboxylic acids as ligands, resulting in high energy consumption and potential pollution during synthesis, which deviates from the principles of green chemistry[3,16]. In recent years, bio-metal-organic frameworks (Bio-MOFs) have demonstrated superior environmental and economic sustainability by incorporating biomass-derived ligands and green solvents. In terms of cost and environment, Bio-MOF synthesis mostly employs one-step reactions with low energy consumption and high yields (70%~85%); the by-products are mainly water or inorganic salts, making post-treatment simple. Taking biomass-derived ligands (such as organic acids obtained from PTA recovery or enzymatic regeneration) as an example, their cost is 1~5 USD/kg, significantly lower than common chemical ligands like H₃BTC (reagent-grade prices can reach tens to hundreds of USD/kg)[22-23], and traditional carboxylic acid ligand modification routes are complex and more costly. Overall, Bio-MOFs are characterized by "renewable raw materials, green solvents, energy-saving processes, and controllable costs," demonstrating superior environmental and economic sustainability over their lifecycle compared to traditional MOF systems.
Currently, various Bio-MOFs exhibit excellent performance in CO2capture, maintaining stable structures and achieving high-selectivity adsorption even under humid gas flow conditions. Some studies have even turned the presence of water vapor into a factor that enhances adsorption performance, providing a new paradigm for CO2capture. This review first summarizes the types of ligands used to construct bio-metal-organic framework materials and the general rules for building bio-MOF hybrid materials; subsequently, it summarizes, analyzes, and discusses the static adsorption behavior of Bio-MOF materials in combination with pore structure types such as pore size and surface functional groups, as well as surface chemical modifications; based on the structural characteristics and effects resulting from the incorporation of biomolecules into MOF materials, it further classifies and summarizes the CO2adsorption applications of derived Bio-MOFs materials; finally, it discusses the challenges and opportunities in the modern technological context for Bio-MOFs materials in the field of CO2capture.

2 Overview of Bio-MOFs

2.1 Basic Definition and Characteristics of Bio-MOFs

MOF materials are coordination polymers with potentially porous open frameworks, primarily formed through the coordination self-assembly of metal ions or metal clusters with bidentate or multidentate ligands.[24]. Bio-metal-organic framework materials are a subclass of MOF materials. Although there is no unified definition for Bio-MOFs, they are generally considered to be crystalline porous materials formed by the self-assembly of biocompatible metal ions and biomolecules. These materials contain at least one biomolecule, emphasizing biocompatibility and biological applications, and the synthesized MOF materials must contain at least one biological molecule.[25-26].
Bio-MOF materials have been applied in various fields such as adsorption separation, catalysis, and drug delivery[27-28], offering numerous advantages: (1) The ligand molecules constituting Bio-MOF materials are mostly derived from renewable resources, which are abundant and low-cost; (2) They can be used to construct MOF materials with different structural types, such as rigid and flexible structures; (3) Biomolecules possess rich coordination chemical sites and self-assembly functions, enabling the functionalization of MOF materials; (4) They are potential candidates for constructing chiral MOF materials, commonly used for the separation and purification of drug molecules; (5) The coordination of diverse biomolecules with different metal ions generates Bio-MOF materials with varying spatial structures, providing more possibilities for material design and application. Biomolecules commonly used to construct Bio-MOFs are shown inTable 1.

2.2 MOFs constructed from biomolecules

The weak binding between metal ions and organic linkers leads to poor stability of MOFs, which easily decompose in water or acidic/alkaline environments, releasing toxic organic ligands and threatening environmental safety[12,19]. Using biomolecules and their derivatives as single linkers to replace traditional organic linkers for synthesizing MOF materials can avoid the toxicity pollution problems caused by the poor stability of conventional MOFs. The ligands used in Bio-MOFs are mostly derived from renewable resources and primarily exist in living organisms, such as amino acids, peptides, nucleobases, porphyrins, and sugars[26-30]. These ligands, especially amino acid molecules, possess various shapes and sizes, contain multiple coordination sites and functional groups, and can be used to control hydrogen bonding and create flexible yet robust MOF structures[20]. The non-toxicity, biocompatibility, and structural diversity of bio-MOFs make them widely applicable in drug delivery[31-32], gas separation[20,33], proton conduction[34], chiral recognition[35], and catalysis[36]and other fields.

2.2.1 Amino Acids (AAs)

In synthesizing amino acid-based MOF materials, controlling structural coordination is crucial. This typically involves two aspects: material properties and synthesis conditions[21,26]. Material properties include: (1) transition metals or clusters and their oxidation states determining coordination; (2) the charge nature of ligands (positive, negative, or zwitterionic) to ensure coordination precision; (3) the number of available binding sites, i.e., the number of O and N atoms available for binding; (4) L- or D- isomeric forms. Synthesis conditions include pH, temperature, pressure, and reaction time. Most importantly, selecting suitable biomolecular ligands for transition metal ions with specific oxidation states. Anderson et al.[26]elaborated in detail on the coordination modes of different biomolecules and their derivatives with various metal ions, as well as the visual representation of the formed bio-MOFs, focusing on the influence of ligand structure on material structure. Qazvini et al.[37]reported a zirconium amino acid metal-organic framework MIP-202(Zr) for proton conduction (Figure 1a), synthesized via a hydrothermal method using Zr4+ metal ions and aspartic acid. This material not only offers the advantages of being green, scalable, and easy to prepare, but also conforms to Pearson's hard and soft acids and bases theory[12,38], exhibiting excellent hydrolytic and chemical stability in aqueous solutions over a wide pH range. At 363 K and 95% relative humidity, MIP-202(Zr) demonstrated a high proton conductivity of 0.011 S/cm, making it one of the candidate materials approaching the commercial benchmark Nafion. Furthermore, Bio-MOFs with amino acids as ligands can provide Lewis acidic metals, basic sites, and hydrogen bonding groups in catalytic reactions, softening reaction conditions[39-40]. AAs-MOFs can serve as precursors for carbon-based composites to construct high-performance batteries. Dong et al.[41]embedded selenium clusters into nitrogen-doped hierarchical radial structured microporous carbon (N-HRMC) constructed using a zinc-glutamate MOF as a precursor, for advanced sodium storage (Figure 1).

2.2.2 Peptide

Peptides are formed by the dehydration condensation of multiple amino acids, possessing a planar structure with at least one free carboxyl group (C-terminal residue) and one free amino group (N-terminal residue), providing favorable conditions for constructing multifunctional MOF materials. Peptide molecules offer numerous advantages when used to synthesize MOF materials[28,43]: Peptides with double-bond characteristics exhibit a higher degree of adaptability, preventing bond rotation; the diversity of peptide structures determines the diversity of MOF materials, and the chiral properties of peptides make them excellent candidates for preparing chiral bio-MOFs. Mantion et al.[44] first reported MOF materials synthesized from tripeptide ligands. In 2017, Navarro-Sánchez et al.[45] reported a chiral Cu(II) 3D MOF based on the tripeptide Gly-L-His-Gly (GHG),Figure 2bandFigure 2c show the spatial structures of the tripeptide molecule and its corresponding MOF, respectively; this is also the first MOF material capable of separating chiral polar drugs (methamphetamine (MA) and ephedrine (EP)) (Figure 2a). Additionally, most peptide molecules, due to their structural flexibility, have become excellent candidates for constructing flexible MOF materials[45].

2.2.3 Nucleic acid

Rich in a large number of oxygen and nitrogen donor sites with different basicities, possessing self-assembly properties, rigid molecular structures, and strong metal and hydrogen bonding capabilities, it is an ideal biological ligand for designing and synthesizing metal-organic frameworks.[26,28]. Due to their environmental friendliness and abundance, a large number of MOF materials are based on nucleobases, such as Bio-MOF-1.[39,47]This series of materials can not only achieve high-performance adsorption of CO2, but also serves as precursors with broad application prospects in the field of catalysis.

2.2.4 Porphyrins

Porphyrins and metallated porphyrin derivatives exist in nature and living organisms as plant and animal pigments (chlorophyll or heme). As widely studied biomolecular ligands, they play important roles in many chemical and biological processes.[20,31,40,48]. Kathalikkattil et al.[49]reviewed synthesis strategies for MOFs based on porphyrins and their derivatives, highlighting applications of porphyrin-based MOFs in biomedical fields such as tumor therapy and biosensing. Porphyrinic MOFs (PMOFs) are widely used in gas separation due to their hollow structures. Shang et al.[48]achieved efficient capture of CO2 from wet flue gas by inserting transition metals into porphyrin-based metal-organic frameworks, demonstrating the potential of PMOFs in environmental remediation. With excellent thermal and chemical stability as well as unique optical properties, PMOFs have become a hot research area.[50].

2.2.5 Natural products

Carboxylic acid ligands are the most commonly used linkers in MOF synthesis. Considering the green sustainability of synthesizing MOF ligands, in addition to the aforementioned biomass-derived organic compounds, natural aliphatic dicarboxylates or polyphenolic green organic compounds can also be selected to construct MOF materials (Table 2). These MOF materials synthesized from natural dicarboxylic acids have been widely applied in separation and catalysis fields, demonstrating the diversity and application potential of Bio-MOFs.[20].

2.3 Derived Bio-MOFs (biomolecule-MOF hybrid structures)

With the advancement and widespread application of MOF synthesis technologies, methods for integrating biomolecules into MOF structures have received increasing attention[27]. Biomolecule-functionalized modification of MOF materials serves as a low-cost and sustainable strategy for preparing advanced functional materials with excellent performance. Among these, the most extensively studied approach involves post-synthetic modification of MOFs using biomolecules as functionalizing agents or modulators[36,51-52]. Subramaniyam et al.[21]systematically introduced the biofunctionalization of MOFs, including structural and functional applications with nucleic acids and amino acid-based biomolecules (such as single amino acids, peptides, and proteins), as well as methods for covalent and non-covalent modification of MOFs. The post-synthetic modification strategy is first based on the preparation of MOF materials, where the initially prepared MOFs possess binding sites (—Cl, —Br, —NH2, etc.) that interact with biomolecules, enabling the preparation of biomolecule-MOF conjugates through these sites. Zhang et al.[53]prepared MIL-101-CM by chloromethylating MIL-101(Cr) and utilized the interaction between —Cl and the —NH2 group of amino acids to synthesize MIL-101(Cr) modified with glycine, histidine, and cysteine. This material not only retained a high specific surface area but also demonstrated excellent uranium adsorption capacity, selectivity, and recyclability in aqueous solutions.
Due to the diversity of porous MOF materials, they can be easily functionalized with naturally available amino acids (or protected amino acids) and alkaline earth metals. Newar et al.[36]reported a natural amino acid-functionalized metal-organic framework for asymmetric alkali metal catalysis (Figure 3a); in the presence of HBTU and diisopropylethylamine (DIEA), the amino groups of pristine UiO-68-NH2 were 100% functionalized via amide coupling with N-Fmoc-protected amino acids; after deprotection of the amino groups, amino acid-grafted UiO-68 MOFs were obtained; subsequently, through multi-step reactions and synthesis with an iron precursor followed by metallation, catalysts for hydrosilylation and hydroboration of carbonyl compounds with high specific surface area, high activity, and enantioselectivity (ee > 99%) were achieved (Figure 3b and Figure 3c).
Furthermore, biomolecule-functionalized MOFs can also be prepared via in situ self-assembly of organic/inorganic precursors with biomolecules. Amino acids are organic ligands containing both carboxyl (—COOH) and amino (—NH2) groups; their organic side chains can confer hydrophobicity or hydrophilicity, existing as polar (e.g., alcohol) or nonpolar (e.g., alkyl chain) side chains. Their rich coordination chemistry (via carboxylates, amino groups, and side chains) makes them a powerful class of organic ligands for functionalizing MOF structures, often serving as secondary ligands to generate three-dimensional frameworks with other primary ligands.[21,26]. Zhao et al.[54]reported a one-pot synthesis of a highly chiral metal–organic framework via ligand in-situ substitution (LIS), where D-histidine (D-His) ligands replaced 2-methylimidazole. This crystalline material features permanent narrow pores, high enantioselective adsorption, and excellent reusability without loss of structural integrity or enantioseparation activity. This LIS strategy, which imparts chirality to achiral MOF structures, not only extends enantioseparation to unexplored microporous materials but also provides a new approach for novel MOF functionalization.

3 CO of Bio-MOFs2adsorption applications

Bio-metal-organic frameworks (Bio-MOFs) in CO2capture exhibit significant advantages over traditional MOFs, primarily due to their unique structural design and optimized performance[46,55-56]. Bio-MOFs are constructed using natural, low-cost, and biocompatible biomolecules (such as nucleobases and amino acids) as organic linkers, thereby endowing the materials with excellent biocompatibility[57]. The structural advantages are reflected in the integration of the inherent specificity of biomolecules (such as molecular recognition and self-assembly capabilities) into the framework[57], enabling the designed adsorbents to combine thermodynamics and kinetics (molecular sieve effect) for highly selective separation (e.g., ZnBTCA exhibits high selectivity in binary gas mixtures). In terms of practical application performance, while many traditional MOFs (such as Mg-MOF-74 and MOF-5) are prone to structural collapse under humid conditions, certain Bio-MOFs (such as adenine-based MOFs and PCN-222) demonstrate superior hydrothermal stability[20], maintaining crystallinity and porosity even after immersion in water or vapor[58-59].

3.1 Classification of CO2adsorption behavior by Bio-MOFs.

Currently, the CO2 adsorption behavior of most constructed Bio-MOF materials is mainly influenced by four factors. (1) Molecular sieving effect[60]: Utilizing size or shape exclusion effects, one or more components of a gas mixture can smoothly enter the pores to be adsorbed while other components are excluded from the pores. (2) Equilibrium sieving effect[61]: Utilizing the differences in interaction forces between the adsorbent and different gas molecules, the target component is preferentially adsorbed. (3) Gate-opening effect[62]: The transition process of flexible MOF materials from a closed-pore phase to an open-pore phase in response to external stimuli (pressure, temperature, or other energy fields), utilizing differences in specific opening pressures to achieve separation of guest molecules. (4) Mixed effect[60,62-63]: A mixed effect combining size exclusion with thermodynamic separation, and size exclusion with the gate-opening effect, which can improve the selectivity and working capacity of microporous MOF materials.

3.2 Bio-MOFs adsorb CO2

Direct synthesis of Bio-MOFs using biomolecules as ligands for CO2capture is the most cost-effective strategy (Table 3). Gu et al.[64]proposed the concept of directly synthesizing ligands and MOFs in a continuous reaction, i.e., starting from biomass sources to linearly synthesize bio-derived ligands (FDCA) (Figure 4a), followed by the in situ synthesis of the MIL-160(Al) and PCN-233 series of MOFs (Figure 4bandFigure 4c). This strategy avoids the tedious and energy-intensive processes of filtering, purifying, or drying intermediate products. Ethane has high polarizability and strong interactions with MOFs; thus, the samples preferentially adsorb ethane, followed by CO2. At 298 K and 1 bar (1 bar = 100 kPa), the adsorption capacity of C2H6in MIL-160(Al) reaches 4.04 mmol/g, whereas that of CH4is only 0.87 mmol/g. The adsorption of CO2is also higher than that of most reported MOFs (Figure 4). It also demonstrates excellent cycling performance and easy regenerability, enabling selective ethane capture under high-humidity conditions, which holds great potential for industrial applications.
MIP-202 (Zr) not only possesses excellent proton conductivity, but its ultra-high CO2 selectivity also makes it stand out among numerous CO2 capture materials. Lü et al.[61]reported the adsorption selectivity of MIP-202 (Zr) for CO2/CH4 and CO2/N2 gas mixtures. The amino groups on the L-aspartic acid ligands do not coordinate with the metal centers, resulting in a high density of amino groups on the inner walls of the MIP-202 channels, which enhances affinity with CO2; MIP-202 has two types of channels, namely large octahedral pores and small tetrahedral pores, with a ratio of large to small pores of 8:5. Simulation calculations indicate that CO2 molecules, which have higher polarizability and quadrupole moments, exhibit strong van der Waals forces and electrostatic interactions with the inner walls of the material channels, preferring to adsorb within the large pores, whereas N2 and CH4 molecules, which have lower polarizability and quadrupole moments, adsorb within the small pores. Furthermore, since there are more large pores than small pores per unit cell, it can be seen that it preferentially adsorbs CO2. In summary, due to these two reasons, MIP-202 exhibits ultra-high CO2/CH4 (72.9 and 241.5 for 50/50 and 10/90, respectively) and CO2/N2 (1.95×106 and 2129.1 for 50/50 and 15/85, respectively) IAST selectivity at 298 K and 100 kPa. Although MOFs have broad application prospects in the field of gas separation, almost all reported MOF adsorbents suffer from a trade-off between adsorption capacity and separation selectivity (i.e., the Trade-off effect), hindering their industrial application[65-66]. Compared with materials such as Mg-MOF-74, MIP-202 (Zr) possesses ultra-high CO2 adsorption selectivity; however, Mg-MOF-74 is selected as an adsorbent due to its open metal sites (OMSs), which provide electrostatic binding sites via p-complexation to achieve high CO2 adsorption capacity. Nevertheless, OMS materials often co-adsorb other gases, leading to poor separation selectivity, and exhibit weak stability in water or sulfides. However, at 298 K and 1 bar, the CO2 adsorption capacity is only 12.5 cm3/g, which is 1/11 of that of Mg-MOF-74 (196.7 cm3/g)[67], demonstrating a trade-off where capacity is sacrificed in pursuit of ultra-high selectivity. MIP-202 is a typical example of capturing CO2 via an equilibrium sieving mechanism, whereas Bio-MOF materials for kinetic sieving of CO2 are rarely reported. Bao et al.[68]reported an ultramicroporous metal-organic framework material constructed based on the biomolecular gallic acid ligand (denoted as M-gallate (M = Mg, Ni, and Co)), with a pore size of 3.52–6.5 Å (1 Å = 0.1 nm), possessing a pore size dimension similar to that of CO2 molecules (Figure 5); at 298 K and 1 bar, it exhibits excellent CO2 adsorption performance, with adsorption capacities in the order of Mg-gallate (5.05 mmol/g) > Co-gallate (4.08 mmol/g) > Ni-gallate (3.91 mmol/g). Among these, the adsorption performance of Mg-gallate is even superior to previously reported MOF materials exhibiting kinetic sieving effects, second only to Mg-MOF-74 (6.2 mmol/g) under the same conditions. Notably, the M-gallate series of materials (e.g., Co-gallate) demonstrate outstanding performance in gas mixture separation, particularly for the separation of C2 substances (Figure 6a~Figure 6d), while also occupying an important position in C4 olefin separation[68-69]. However, although Bio-MOFs are composed of green ligands, most Bio-MOF materials still suffer from poor water vapor stability and moderate adsorption capacity under flue gas conditions. For instance, for most MOF materials under humid conditions, competitive adsorption of H2O may severely reduce CO2 capture capacity, and materials that are thermally unstable and sensitive to moisture may undergo structural collapse under harsh conditions. Engineering modification is another important task to improve their stability and adsorption performance in practical applications. Currently, there are the following two methods to improve the CO2 adsorption performance of Bio-MOF materials.

3.2.1 Amino functionalization of ligand molecules

CD-MOFs are hydroxyl-rich porous network structures composed of naturally recyclable cyclodextrin (CD) and alkali metal ions (K+, Na+, Rb+, and Cs+). The Stoddart group[71]has presented the crystal structure of γ-CD-MOF and explored its CO2capture performance, finding that the free hydroxyl groups present on the material give it strong selective adsorption capacity for CO2at low pressure. Li et al.[72]reported two types of isostructural MOFs based on γ-CD, finding that the selectivity for CO2/C2H2can reach 118.7 at room temperature. Although γ-CD-MOF exhibits high adsorption performance for CO2under certain conditions, its structure is particularly sensitive to water, collapsing even in air, and the high cost of γ-CD severely limits its application. Hartlieb et al.[73]proposed a method to synthesize mono-amino functionalized CD-MOFs (NH2-CD-MOF-2) using an asymmetrically substituted γ-CD. The resulting material exhibits strong adsorption capacity for CO2at low pressure, indicating the presence of a chemisorption process; carbonate functional groups form on the free hydroxyl groups on the primary face, followed by a physisorption process at elevated pressures. Xu et al.[46]adopted a similar method to substitute the hydroxyl group at the CFigure 6a) C6position of inexpensive β-CD (Figure 6b) with a tosyl group (6-OTs-β-CD) (2-β-CD (Figure 6c), utilizing the better leaving ability of p-toluenesulfonyl to undergo a substitution reaction with ammonia, forming 6-NHFigure 6d), successfully introducing amino groups into the CD-MOF structure (2-β-CD-MOF to achieve a dual effect of chemisorption and physisorption, while enhancing the water resistance of CD-MOFs and their CO2adsorption capacity (10 times that of β-CD-MOF), exhibiting significant CO2/N2adsorption selectivity performance (SIAST=947.52) (Figure 6eandFigure 6f).

3.2.2 Ion exchange

In PSM strategies for improving the gas adsorption performance of MOF materials, most studies have focused on modifying organic ligands. In addition, ion exchange strategies have gradually attracted researchers' attention. Ion exchange is divided into cation exchange[74-75]and anion exchange[76], which can significantly improve the applications of MOFs in various fields (catalysis[65], ionic conductivity[66]and separation[67]). An et al.[39]demonstrated that post-synthetic exchange of extra-framework cations in the anionic Bio-MOF-1 (Zn8(ad)4(BPDC)6O·2Me2NH2) can serve as a means to systematically adjust pore size and aperture, and utilized this strategy to optimize its CO2adsorption performance. Meanwhile, due to its ion exchange characteristics, it was selected as a "proof-of-concept" model. The adenine ligands provide N-rich basic sites (including pyrimidine and amino groups), and these modified channels help enhance affinity for CO2and high-selectivity capture. Pan et al.[67]confirmed that Me2NH2+cations, as counterions in the Bio-MOF-1 channels, are easily exchanged with K+. They prepared N-doped porous carbon materials based on MOFs through one-step carbonization of pristine bio-MOF-1 and K@bio-MOF-1 (K+-exchanged bio-MOF-1). After K+ion exchange, the microporosity of the carbon material was improved, exhibiting good CO2adsorption performance (4.75 mmol/g) at 298 K and 1 bar, as well as high adsorption selectivity for CO2/N2(Sads=99.1). This strategy uses the MOF structure as an N source and a self-sacrificing template, and utilizes cation exchange to pre-regulate the pore environment, representing an efficient and unique method for preparing high-performance carbon-based adsorbents. Ma et al.[77]broke the long-standing limitation that CD-MOFs are constructed only by large cations, achieving partial substitution of K+by Li+through co-crystallization of K+and Li+without destroying the porous structure of CD-MOFs. Although the CO2adsorption capacity of Li/K-CD-MOF (4.5 mmol/g) increased only slightly compared to CD-MOF-1 (4.2 mmol/g), this demonstrates that partial cation exchange allows fine-tuning of the local microenvironment of the MOF framework, thereby achieving targeted modulation of gas adsorption performance. Recently, Svensson et al.[74]proposed a highly porous and stable zirconium-ellagic acid framework (SU-102) synthesized from ellagic acid (Figure 7). The synthesis of SU-102 highlights the possibility of preparing stable, high-performance multifunctional materials from plant-based components derived from sustainable sources. This work validates the significant impact of regulating the pore chemical environment via cation exchange on gas adsorption performance. After the dimethylammonium (DMA) cations were exchanged with Na+, its specific surface area increased from 472 m2/g to 573 m2/g; most notably, SU-102 exchanged with K+(K+) significantly enhanced CO2uptake capacity, increasing from 27 cm3/g (Figure 7e) to 90 cm3/g (Figure 7f) at 293 K and 1 bar, while the CO2/N2selectivity increased from 12 to 81. This powerfully demonstrates that in biomolecule-based anionic bio-MOF frameworks, simple cation exchange can achieve synergistic optimization of CO2/capture performance (simultaneous improvement in capacity and selectivity).

3.3 Derived Bio-MOFs CO2adsorption

Although directly constructing MOF materials from biomolecules for carbon capture has many advantages, their adsorption performance is poorer compared to MOF materials constructed with other ligands. Synthesizing chiral biomolecule-based MOF materials remains challenging and their numbers are limited, so functional modification of existing MOF materials has become a research hotspot (Table 4). Research on improving the CO2 adsorption performance of MOF materials mainly focuses on generating open metal sites or ligands functionalized with Lewis basic groups. Due to the strong interaction between CO2 and basic amino functional groups, amino-functionalized MOFs for CO2 capture have attracted widespread attention[36,42,46,90]. Amine functionalization is a major strategy to enhance the interaction between MOF materials and gas molecules. Common methods for amino functionalization of MOFs include: using carboxylic acid ligands containing amino groups[91-92] and post-synthetic amine modification (PSM) [51,93]. Biomolecules such as amino acids and nucleobases not only possess low toxicity, renewability, biodegradability, and environmental friendliness, but their special reactive groups including amino, carboxyl, and guanidino groups also provide prerequisites for constructing MOF materials with high adsorption performance, making them preferred materials for amino-functionalized MOFs[51,94-95]. When functionalizing traditional MOF materials with biomolecules, the interactions of adsorption sites such as N—H, N—N, —NH2, and C—H are the main driving forces for efficient adsorption and selective separation of CO2[85]. The following categories are often used for functionalized MOF materials adsorbing CO2.

3.3.1 Structural defects

Defect engineering has recently become a new trend for tuning the physicochemical properties of metal-organic frameworks (MOFs)[96]. In MOF materials where functionalization is difficult to introduce, constructing defective MOFs can provide favorable conditions for the entry of functional linkers. Post-synthetic exchange (PSE) and modulated synthesis are currently the two commonly adopted methods for creating structural defects in defect-engineered MOF materials[97]. The most direct method to generate defects in MOF materials is modulated synthesis using coordination modulators, which involves adding super-stoichiometric amounts of monocarboxylic acids (typically formic acid, acetic acid, or benzoic acid) as modulators; these compete with polycarboxylate linkers for coordination to metal clusters[52,98]. In principle, any species containing at least one carboxyl group, provided its size does not exceed the cavity created by missing-cluster defects, can be used for functionalizing and modifying defective MOFs. On the other hand, functional modulators must be well-defined in terms of length and geometry to be incorporated into a defect-free framework, but this also limits the range of functional groups that can serve as modulators. Among the available monocarboxylic acid modulators with functional properties, small-molecule amino acids, as a class of green, non-toxic natural products rich in basic groups that interact strongly with CO2, are gradually receiving widespread attention. Introducing structural defects using biomolecules can enhance the adsorption and catalytic capabilities of MOF materials. Gutov et al.[99]added functionalizing agents to terephthalate linkers to achieve biological or catalytic properties in MOFs, using L-proline, glycine, and L-phenylalanine as pre-modulators to texture the cavity environment of UiO-66-type zirconium-based MOFs. The glycine molecules point towards the cavities, thereby leading to an increased specific surface area and demonstrating a higher capture capacity for CO2 molecules. Shearer et al.[100]investigated the possibility of functionalizing UiO-66 with amino acids and generating defects in UiO-66 via PSE (Figure 8a); experiments indicated that the best method for functionalizing UiO-66 is to add benzoic acid as a modulator prior to the synthesis of the UiO-66 precursor to synthesize "50Benz" with a high concentration of cluster defects. After removing the benzoate ligands with hydrochloric acid, successful incorporation of L-serine occurs (Figure 8b).
During testing of CO2capture performance, it was found that as the degree of L-serine functionalization increased, the CO2/N2adsorption selectivity also improved accordingly. This study indicates that the reactivity of UiO-66 depends not only highly on the presence of defects but also highly on the type of compensating ligands, providing a new approach for the functionalization of Zr-MOFs. In another modification study targeting Zr-MOFs, Zhu et al.[101]successfully anchored green, non-toxic L-arginine onto the MOF-808 inorganic clusters using a solvent-assisted ligand incorporation method for high-performance CO2/C2H2mixture separation under humid conditions. Furthermore, this study transformed the negative impact of water in the gas mixture into a positive promoting effect, offering a new paradigm for the separation of CO2/C2H2.

3.3.2 Functional modification

To achieve high-performance adsorption of CO2 molecules, Lü et al.[51] obtained a series of MOF-808-AAs with different adsorption capacities for CO2 through post-synthetic modification of the robust MOF-808 system using amino acids (Figure 9a). As shown in Figure 9b, a multi-step synthesis method was employed: first, microcrystalline MOF-808 was synthesized, then treated with hydrochloric acid (HCl) to remove formate (HCOO-) ligands, yielding the secondary building unit structure MOF-808-FR, and finally, 11 types of amino acids (Figure 9c) were loaded onto MOF-808-FR, producing a series of MOF-808-AAs.
When functionalized with amino acids, the carboxylates of MOF-808 bind directly to Zr(IV) centers, creating pores capable of selectively adsorbing CO2 from flue gas. Adsorption results for CO2 under flue gas conditions show (Figure 9d) that MOF-808 functionalized with glycine (Gly) and D/L-lysine (DL-Lys) (MOF-808-Gly and -DL-Lys) exhibit the highest uptake capacity for CO2. This is because, after functionalization, the amine residues of the amino acid units point toward the interior of the MOF pores, giving them sufficient affinity for CO2 in the presence of water (Figure 9e), thereby enabling the formation of bicarbonates as well as carbamates and carbamic acid (Figure 9f). This chemical nature endows MOF-808-AAs with adsorption-desorption characteristics for CO2 under mild conditions. This study reveals how amino acids bind to the MOF backbone to construct internal pore surface chemistry, thereby achieving CO2 binding and release without heating under mild conditions, greatly enhancing our understanding of carbon dioxide chemistry in MOFs. In another modification study on UiO-66, Ma et al.[91] developed a mild acetic acid-assisted polyhydroxy acid modification strategy for UiO-66 to improve CO2 adsorption levels. D-gluconic acid (GA), which possesses multiple hydroxyl groups, replaces the acetic acid coordinated at the metal nodes of UiO-66 through competitive coordination, allowing the coexistence of hydrogen bond donors and Lewis acid sites. Compared with pristine UiO-66, GA-modified UiO-66 achieves a maximum CO2 adsorption capacity of up to 108 cm3/g (273 K, 1 bar) and 76 cm3/g (298 K, 1 bar), far exceeding that of UiO-66.

3.3.3 Protect open metal sites (OMS)

In practical applications, hydrothermally stable MOF materials are required, but obtaining stable MOFs under water or humid conditions is challenging, especially for MOFs with open metal sites (OMS) (e.g., Cu-BTC, M-MOF-74, etc.). This is due to the strong affinity of OMS for water molecules, causing water molecules to accumulate near the OMS under continuous hydration, leading to the displacement of ligands from the OMS.[92], a direct method to solve this problem is to protect the OMS within the porous structure. Al-Janabi et al.[102]reported a post-synthetic modification (PSM) method to prepare glycine-doped Cu-BTC MOF. When evaluating the single-component gas (CO2 and N2) adsorption and dynamic water vapor adsorption performance, it was found that doping with glycine, which contains amino and carboxyl groups, can saturate the OMS in the parent Cu-BTC MOF, thereby improving the material's hydrothermal stability and CO2/N2selectivity. In another study, Sran et al.[103]adopted a low-energy hydroxy double salt method to successfully introduce glycine (HKUST-1-UF-GLY0.3) into the rapidly synthesized HKUST-1-UF (Cu-BTC) material for efficient separation of CO2/C2H2. The study showed that HKUST-1-UF-GLY0.3 exhibited more favorable adsorption sites for C2H2 and also enhanced the material's moisture resistance. Generally, in post-synthetic modification methods, the binding of amino molecules to unsaturated metal centers is an effective approach; while regulating the pore structure of MOF materials, it can further improve the water stability of MOFs with unsaturated metal sites. However, the number of MOFs possessing this capability is very limited, which can be attributed to the low capacity of metal nodes and structural stability.[100].

4 Conclusion and Outlook

MOF materials in CO2 adsorption have demonstrated immense potential. Through rational chemical and pore structure design, efficient adsorption of CO2 can be achieved under flue gas conditions. However, the synthesis of most existing MOF materials relies on organic linkers derived from fossil fuels, without considering the greenness of the linkers during their synthesis, as well as the potential for low adsorption capacity and toxic linker leakage when applied to CO2 adsorption.
Bio-MOFs exhibit tremendous application potential in CO2 adsorption due to their green and abundant ligands rich in special active sites. Based on this, this article, oriented towards CO2 adsorption, summarizes Bio-MOFs synthesized from naturally available biomolecules such as amino acids, peptides, nucleobases, porphyrins, and natural products, as well as methods for functionalizing existing MOF materials with biomolecules, and applies them to CO2 adsorption under flue gas conditions and the purification of hydrocarbons. Direct synthesis of MOFs from biomolecules is the most economical strategy, but high-performance CO2-adsorbing Bio-MOFs are scarce and difficult to meet practical applications; therefore, this article presents two methods to enhance the CO2 adsorption performance of Bio-MOF materials. Furthermore, it focuses on incorporating biomolecules with special functional groups into existing MOF materials to form composite bio-MOFs, and summarizes three types of functional composite Bio-MOF materials used for CO2 adsorption.
Currently, MOF materials have been widely applied in CO2 adsorption; however, when MOF materials are used for adsorbing CO2, a trade-off effect exists among adsorption performance. Especially under humid conditions, issues such as reduced adsorption capacity, structural degradation, and poor selectivity of MOF materials arise, severely hindering their industrial application. How to break this effect is a key focus of future research. Secondly, in an era of explosive growth in MOF materials, utilizing appropriate force fields and algorithms to screen tens of thousands of MOF materials through quantum mechanical calculations, DFT calculations, machine learning, and high-throughput computations (GCMC) to identify those that remain green, highly adsorptive, and multifunctional even under complex operating conditions holds significant scientific value for guiding the design and synthesis of future high-performance MOF materials. Additionally, DAC technology is gradually gaining attention, yet current porous adsorbent materials constrain its large-scale application. It is believed that with the advancement of science and technology, interdisciplinary approaches can be leveraged to develop multifunctional MOF materials capable of achieving CO2 efficient capture and utilization.

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Funding

Foundation Central Government for Reform and Development of Local Universities， the Basic Research Support Program for Outstanding Young Teachers of Heilongjiang Provincial Department of Education(YQJH2024049)

“Excellent Master’s and Doctoral Dissertations in Longjiang in the New Era”(LJYXL2024-030)

Joint Funds of National Natural Science Foundation of China(U24B6004)

National Natural Science Foundation of China(52200091)

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