The efforts to achieve sustainable chemical conversion and efficient CO utilization are critical to addressing climate change and environmental sustainability, and therefore the development of effective CO conversion catalysts is crucial. In this study, novel acid-base bifunctional catalysts, MIL-101-SOH@Atz and MIL-101-SOH@DAtz, were successfully synthesized using MIL-101-SOH as an acid support material through post-synthetic modification with 3-amino-1,2,4-triazole (Atz) and 3,5-diamino-1,2,4-triazole (DAtz) for CO conversion reaction. The incorporation of the amine species into MIL-101-SOH created unique synergistic effects with dual acid-base catalytic sites, facilitating the efficient conversion of CO and epoxides into cyclic carbonates. Among the catalysts, MIL-101- SO3H@DAtz demonstrated superior catalytic performance with achieving 100% epichlorohydrin (ECH) conversion with over 99% selectivity to cyclic carbonate with high selectivity of > 99% under the ambient condition of 1 bar CO without any co-catalyst or solvent. The elucidated CO cycloaddition reaction mechanism highlights the synergistic effects of acid-base functionalities and CO-philic Lewis bases as well as hydrogen bonding donor groups, providing valuable insights into the factors contributing to superior catalytic performance. The simulated flue gas (15% CO/85% N, v/v) was also conducted using MIL-101-SOH@DAtz catalyst. Additionally, the MIL-101-SOH@DAtz catalyst exhibited remarkably robust structural stability and recyclability, maintaining its activity over multiple cycles.

中文翻译：

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通过在 MIL-101-SO3H 催化剂上接枝胺来提高温和条件下 CO2 环加成的催化性能

实现可持续化学转化和高效二氧化碳利用的努力对于应对气候变化和环境可持续性至关重要，因此开发有效的二氧化碳转化催化剂至关重要。本研究以MIL-101-SOH为酸载体材料，通过3-氨基的合成后修饰，成功合成了新型酸碱双功能催化剂MIL-101-SOH@Atz和MIL-101-SOH@DAtz。 -1,2,4-三唑 (Atz) 和 3,5-二氨基-1,2,4-三唑 (DAtz) 用于 CO 转化反应。将胺类物质纳入 MIL-101-SOH 中，与双酸碱催化位点产生独特的协同效应，促进 CO 和环氧化物有效转化为环状碳酸酯。在这些催化剂中，MIL-101-SO3H@DAtz表现出优异的催化性能，在1巴CO环境条件下，没有任何CO，环氧氯丙烷(ECH)转化率达到100%，对环状碳酸酯的选择性超过99%，选择性> 99%。 -催化剂或溶剂。阐明的CO环加成反应机理突出了​​酸碱官能团和亲CO路易斯碱以及氢键供体基团的协同效应，为了解促成优异催化性能的因素提供了有价值的见解。模拟烟气（15% CO/85% N，v/v）也是使用 MIL-101-SOH@DAtz 催化剂进行的。此外，MIL-101-SOH@DAtz 催化剂表现出非常强大的结构稳定性和可回收性，在多个循环中保持其活性。