The CO2 cycloaddition reaction effectively mitigates the greenhouse effect while producing high-value cyclic carbonates. Metal-organic frameworks (MOFs) have shown promise for CO2 cycloaddition with epoxides; however, the aggregation of MOFs due to high surface energy hinders mass transfer and catalytic performance. By pre-coordinating graphene oxide (GO) to regulate the dispersion of MOF-808, the resulting MOF-808/GO-100 composite catalyst exhibits twice the activity of pristine MOF-808, achieving 92.6% conversion of epichlorohydrin (ECH) with 98.2% selectivity to ECH carbonate without adding any co-catalysts. The incorporation of GO introduces numerous hydroxyl groups on the catalyst surface, serving as hydrogen bonding donors. The oxygen-containing groups on GO can compete with ligands for Zr coordination, generating defective Zr sites. The synergistic effect between defective Zr sites and hydrogen bonding donors collectively promotes epoxide opening. Notably, GO correspondingly enhances the dispersion of MOF-808 and induces mesopore formation through its stacking effect at the interface with MOF-808. Across various epoxide cycloaddition reactions, MOF-808/GO-100 consistently demonstrated optimal performance and maintained high stability over multiple reaction cycles.

中文翻译：

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使用高活性和稳定的 MOF-808/GO 复合催化剂通过环氧化物环加成固定 CO2


CO2 环加成反应有效减轻温室效应，同时产生高价值的环状碳酸盐。金属有机框架 （MOF） 已显示出与环氧化物进行 CO2 环加成反应的前景;然而，由于高表面能导致的 MOF 聚集阻碍了传质和催化性能。通过预配位氧化石墨烯 （GO） 来调节 MOF-808 的分散，所得的 MOF-808/GO-100 复合催化剂的活性是原始 MOF-808 的两倍，在不添加任何助催化剂的情况下，实现了 92.6% 的环氧氯丙烷 （ECH） 转化率和 98.2% 的对 ECH 碳酸酯的选择性。GO 的掺入会在催化剂表面引入许多羟基，作为氢键供体。GO 上的含氧基团可以与配体竞争 Zr 配位，产生有缺陷的 Zr 位点。有缺陷的 Zr 位点和氢键供体之间的协同作用共同促进了环氧化物的开放。值得注意的是，GO 相应地增强了 MOF-808 的分散性，并通过其在与 MOF-808 界面上的堆积效应诱导中孔形成。在各种环氧化物环加成反应中，MOF-808/GO-100 始终表现出最佳性能，并在多个反应循环中保持高稳定性。