Aiming at meeting the global goals established for carbon dioxide (CO2) reduction, carbon capture and storage (CCS) plays a key role. In this framework, the adsorption-based CO2 post-combustion cap...

Adsorption of Carbon Dioxide for Post-combustion Capture: A Review

Nowadays, global warming is becoming more and more serious, while CO2 capture technologies have emerged endlessly, with methods of solid-phase CO2 capture for physical adsorption and liquid-phase CO2 capture for chemical absorption. Biochar has been widely used to achieve CO2 sequestration and emission reduction as a result of its wide range of precursor sources, strong adsorption, and rich surface functional groups. It reviews the existing post-combustion CO2 capture solutions, focusing on the analysis of CO2 capture technologies based on liquid-phase ammonia/monoethanolamine and solid-phase carbon-based materials. The former (liquid phase) is with limitation of capture efficiency as a result of strong volatility and thermal degradation, while the latter (solid phase) is accompanied by limited CO2/N2 selectivity. The realization of synergy between the two would “learn from each other’s strengths” to improve the CO2 adsorption ability. The review puts forward the concept of “biochar-functionalized cross-linking synergistic ammonia CO2 capture technology”, which not only broadens the idea of multi-level utilization of biochar, significantly improving the liquid-phase (ammonia) CO2 capture efficiency, but also has practical significance for the utilization of biomass waste and reduction of CO2 emissions. 

Functional Biochar Synergistic Solid/Liquid-Phase CO2 Capture: A Review

The anaerobic fermentation gas (AFG) with CO2 removed is a sustainable energy resource, and converting CO2 in AFG to value‐added chemicals can kill two birds with one stone. Herein, an ionic porous organic polymer (IPOP‐3) catalyst, with triply synergistic effect of its hydroxide anions, nitrogen activation sites and porous structure, is synthesized. IPOP‐3 exhibits an excellent ability to enrich and convert 50 vol.% CO2 by the reactions with various amines into corresponding formamides. The catalyst is also successfully applied to the N‐formylation of CO2 in AFG, and can be easily recovered and reused. The plausible mechanism for the catalytic N‐formylation is proposed. The hydroxide anion in IPOP‐3 activates the Si−H bond of phenyl silane which reacts with the captured CO2 to form formate anion to facilitate the subsequent conversion into formamide. Our work provides a new idea for the purification of AFG and the resource utilization of CO2.

Effective N‐formylation of Amines with CO2 in Anaerobic Fermentation Gas Catalyzed by Triply Synergistic Effect of Ionic Porous Organic Polymer

The direct utilization of diluted CO2 skips the additional enrichment and purification operations required for high-purity CO2, making it shine in the green catalytic process. However, achieving diluted CO2 cycloaddition coupling transesterification with epoxide and methanol over poly(ionic liquids) catalyst and understanding the relevant mechanism at the molecular level are still challenging. Here, a novel porous sulfonyl binuclear carbonate poly(ionic liquid)s (SC-PILs) were successfully prepared by the integration of acidic monomers pre-polymerization with basic anions post-etching, regulating the chemical property of free anions and increasing the specific surface area of copolymerized materials. Relying on the synergy of the built abundant pores and the exposed basic anions, SC-PILs could one-pot efficiently catalyze the cycloaddition coupling transesterification reaction of the simulated flue gas (15% CO2 + 85% N2) without any co-catalyst, and dimethyl carbonate (DMC) with the yield of 80% was obtained. Theoretical studies deeply understood the activation difference of binuclear CO32− anion on CO2 compared with mononuclear CH3COO− anion and the ring-opening mechanism of [CO32−+CO2] adduct on epoxides, providing a better choice for high-value utilization of diluted CO2 from flue gas. 

Porous sulfonyl binuclear carbonate poly(ionic liquid)s for one-pot fixation of diluted CO2 into dimethyl carbonate

CO2 Post-combustion Capture: A Critical Review of Current Technologies and Future Directions

Insight into the reversible behavior of Lewis–Brønsted basic poly(ionic liquid)s in one-pot two-step chemical fixation of CO2 to linear carbonates

Nitrogen-doped microporous carbon using carboxylic acid-functionalized imidazole-type polymers (PDVA) as a carbon precursor was fabricated by a one-step carbonization method without an additional activator. The introduction of acrylic acid was beneficial to promote the formation of microporous structures during the pyrolysis process. By changing the carbonization temperature, the textural properties and surface nitrogen content of the carbon materials were tuned. The synergistic effect of the microporous structure and basic nitrogen sites was conducive to enhancing the CO₂ adsorption performance of porous carbon materials. The CO₂ adsorption quantity of PDVA-C-800 obtained without an additional activator reached 3.18 mmol·g–¹ under 1 bar at 25 °C, which was comparable to that of the reported carbon materials. Besides, PDVA-C-800 possessed excellent cycle stability and recyclability. The fabrication of microporous nitrogen-doped carbon derived from carboxylic acid-functionalized imidazole-type polymers provided an original idea for CO₂ uptake.

Nitrogen-Doped Microporous Carbon Prepared by One-Step Carbonization: Rational Design of a Polymer Precursor for Efficient CO2 Capture

The construction of defects in semiconductor photocatalysts, as a kind of modification methods, plays an indispensable role in the enhancement of the photocatalytic performance. Herein, nitrogen defects were successfully introduced into the framework of graphite carbon nitride (CN-Tx) through thermal polymerization with melamine and 1,2,4-triazole as precursors. The existence of nitrogen defects in CN-Tx were confirmed to be located at the two-coordinated (N2c) C N–C lattice sites, which resulted in the destruction of its planar structure and the initiation of n-π∗ electron transition that greatly expanded the response range to visible light and improved the separation efficiency of photogenerated charge carrier. More significantly, CN-Tx could enhance photocatalytic water purification activity towards different kinds of pollutants. The photocatalytic rates of CN-T3 were estimated to be 2.54 (tetracycline) and 2.31 (2-hydroxynaphthalene) times higher than those of pristine g-C3N4. Furthermore, the possible photocatalytic degradation mechanism over CN-Tx photocatalyst was proposed by free radical trapping experiments combined with ERS characterization. This work provides an in-depth understanding of the important role of nitrogen defects in the electronic structure and chemical properties of g-C3N4 and its photocatalytic water purification performance.

One-step fabrication of nitrogen-deficient carbon nitride through pyrolysis of melamine and 1,2,4-triazole for its enhanced photocatalytic degradation

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Insight into the reversible behavior of Lewis–Brønsted basic poly(ionic liquid)s in one-pot two-step chemical fixation of CO2 to linear carbonates

Nitrogen-Doped Microporous Carbon Prepared by One-Step Carbonization: Rational Design of a Polymer Precursor for Efficient CO2 Capture

One-step fabrication of nitrogen-deficient carbon nitride through pyrolysis of melamine and 1,2,4-triazole for its enhanced photocatalytic degradation