碳酸乙烯酯选择氢解制甲醇/乙二醇双金属催化体系的构建及反应机理研究

CO2经碳酸乙烯酯氢解制备甲醇/乙二醇是典型的原子经济反应，对于碳资源循环利用具有重要意义。本项目拟针对目前碳酸乙烯酯氢解过程中多相催化剂活性较低、反应机理不明确等研究难题，拟采用Ru-Cu簇合物前驱体,经低温固载活化方法制备CeOx负载Ru-Cu双金属催化剂，获取高效选择氢解Ru-Cu/CeOx催化体系；利用in-situ XRD、XPS、Raman、STEM、DRIFT、EXAFS等表征手段，明确催化剂制备参数、CeOx载体表面化学性质对Ru-Cu双金属颗粒尺寸、金属-氧化物载体界面效应的影响规律；系统研究氢解反应条件，阐明Ru-Cu/CeOx微观结构与催化性能的内在关系；结合量子化学/分子力学模拟计算，揭示反应物碳酸乙烯酯/H2在催化剂表面吸附方式、反应中间体等微观机理。本项目对于CO2经碳酸乙烯酯氢解制备大宗化学品甲醇/乙二醇具有重要的理论指导意义和实际应用价值。

The hydrogenolysis of ethylene carbonate derived from CO2 to produce methanol and glycol is a typical atom-efficiency reaction, which is very important for the recycling utilization of carbon source. So far, the catalyst performance is still unsatisfactory and the reaction mechanism is still unclear. This project aims to use Ru-Cu cluster compounds and immobilization method for the preparation of highly efficient Ru-Cu/CeOx bimetallic catalyst system. The effect of preparation method and the chemical properties of CeOx surface on the size of Ru-Cu particals and the interfacial effect between the metal and support will be studied by means of in-situ XRD, XPS, Raman, STEM, DRIFT, EXAFS, etc. A detailed study of catalytic hydrogenolysis performance will be conducted to disclose the structure-activity relationship. Furthermore, in combination with the quantum chemical/molecular mechanics calculations, the microscopic mechanism about the adsorption mode and the key intermediate species involved during the hydrogenolysis of ethylene carbonate will be revealed. The implementation of the project for the selective hydrogenolysis of ethylene carbonate derived from CO2 has great significance in the fundamental research and practical application in the production of bulk chemicals methanol/glycol.