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    骨架结构与碳复合共调控提升催化剂对CO2的吸附与催化转化

    Synergistic modulation of MOFs structure and carbon complex to enhance the integrated CO2 adsorption and catalytic conversion

    • 摘要: 工业烟气中CO2捕获与一体化催化转化是当前的研究热点,金属有机骨架(MOFs)材料在CO2吸附分离领域得到了广泛应用。为了改善铜基金属有机骨架吸附催化剂的耐水稳定性,采用模板剂(AspCuTEA)调控MOFs合成。使用AspCuTEA与碳气凝胶(CCA)复合共调控复合吸附催化剂(AspCuTEA-CCA)结构,提升CO2吸附与催化转化性能。在循环固定床中,AspCuTEA-CCA用于CO2吸附分离后,直接与环氧氯丙烷进行环加成反应制备环状碳酸酯。吸附结果表明:AspCuTEA-CCA对纯CO2和15%CO2的饱和吸附量达到386 mg/g和198 mg/g,在少量水存在的情况下能促进CO2的吸收。吸附后的CO2直接催化转化为环状碳酸酯的转化率达到93.6%。10次吸脱附循环和3次的催化转化循环不影响AspCuTEA-CCA结构,AspCuTEA-CCA表现出了良好的结构稳定性和吸附催化稳定性,具有工业化应用的潜力。

       

      Abstract: The integrated capture and catalytic conversion of CO2 from industrial flue gas is a current research focus. Metal-organic frameworks (MOFs) are widely used in CO2 adsorption and separation. To enhance the water stability of a copper-based MOF adsorbent-catalyst, a structure-directing agent (AspCuTEA) was employed to modulate its synthesis. This AspCuTEA was further integrated with hydrophobic carbon aerogel (CCA) to co-regulate the structure of a composite adsorbent-catalyst (AspCuTEA-CCA), aiming to improve its performance for both CO2 adsorption and conversion. In a cyclic fixed-bed system, the AspCuTEA-CCA was first used for CO2 adsorption and separation. Subsequently, the adsorbed CO2 was directly utilized for the cycloaddition reaction with epichlorohydrin to produce cyclic carbonate without a desorption step. Adsorption results showed that the AspCuTEA-CCA achieved saturated CO2 capacities of 386 mg/g for pure CO2 and 198 mg/g for a 15% CO2 mixture. Notably, the presence of a small amount of water vapor enhanced CO2 uptake. The direct catalytic conversion of the adsorbed CO2 into cyclic carbonate reached a yield of 93.6%. The AspCuTEA-CCA maintained its structural integrity over 10 adsorption-desorption cycles and 3 catalytic conversion cycles, demonstrating excellent structural stability and consistent performance, indicating promising potential for industrial application.

       

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