Covalent Cross‑Linking Strategy for Enhancing the Stability of IL@MOF Composites for Efficient CO2/C2H2 Separation

doi:10.6023/A26010035

Abstract

The separation of carbon dioxide (CO₂) and acetylene (C₂H₂) using solid adsorbents represents a viable approach for producing C₂H₂ in industrial applications. To address the issues of ionic liquid (IL) leaching and limited stability in IL-incorporated metal-organic framework (MOF) composites, we developed a strategy involving the covalent crosslinking of the IL using a diepoxy crosslinker. The covalent cross-linked network not only effectively restricts the migration and leaching of ionic liquids on the MOF surface but also enhances the overall chemical and thermal stability of the composite material. Specifically, this strategy is based on the ring-opening polymerization reaction between the epoxy groups on the cross-linker (ethylene glycol diglycidyl ether) and the amine groups on the ionic liquid ([TEPA][Py], where [TEPA] is tetraethylenepentamine and [Py] is pyrazole). This constructs a stable covalent network within the ionic liquid, which is then firmly anchored onto the surface of ZIF-8 to form a core-shell structured adsorption separation material for CO₂/C₂H₂ separation. Although the crosslinked composite exhibited a lower CO₂ uptake (63.75 cm³ g^-1) compared to its non-crosslinked counterpart (80.29 cm³ g^-1), it maintained considerable adsorption capacity alongside high CO₂/C₂H₂selectivity (>10⁴). The thermal stability of the composites was evaluated by thermogravimetric analysis (TGA). The results show that the crosslinked ionic liquid composite retained a larger mass at a given temperature compared to the pristine composite, demonstrating its enhanced thermal stability.The cross-linked adsorbent exhibited exceptional retention of its adsorption capacity over five consecutive adsorption-desorption cycles, with a negligible capacity loss of less than 0.6%. This performance stands in striking contrast to the severe degradation observed for the non-crosslinked composite, which suffered a rapid capacity loss of over 17% under identical conditions, providing direct evidence for the successful suppression of IL leaching. Finally, dynamic breakthrough experiments conducted under mixed-gas conditions confirmed the exceptional CO₂/C₂H₂separation performance and practical potential of the developed cross-linked IL@MOF composite.

Key words: Composites, Gas Separation, CO₂ Capture, Crosslinking, Stability

Cite this article

Feng Chaoyue, Xue Bo, Che Guoqiang, Liu Dahuan. Covalent Cross‑Linking Strategy for Enhancing the Stability of IL@MOF Composites for Efficient CO₂/C₂H₂ Separation[J]. Acta Chimica Sinica, doi: 10.6023/A26010035.

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共价交联策略强化CO₂/C₂H₂高效分离用IL@MOF复合材料的稳定性^★

Covalent Cross‑Linking Strategy for Enhancing the Stability of IL@MOF Composites for Efficient CO₂/C₂H₂ Separation

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共价交联策略强化CO2/C2H2高效分离用IL@MOF复合材料的稳定性★