碱性纳米碳材料负载钯基双金属催化剂的制备、结构调控及催化效应

项目名称： 碱性纳米碳材料负载钯基双金属催化剂的制备、结构调控及催化效应

项目编号： No.21306203

项目类型： 青年科学基金项目

立项/批准年度： 2014

项目学科： 化学工业

项目作者： 韩军兴

作者单位： 中国科学院过程工程研究所

项目金额： 25万元

中文摘要： 钯基催化剂具有优异的催化性能，但是价格昂贵，因此开发高效、低负载量的钯基催化剂是一项非常具有挑战性的研究工作。本项目以醇醛一步氧化酯化制备甲基丙烯酸甲酯(MMA)工艺在工业化推广过程中遇到的金属钯用量大、催化剂成本高这一难点问题为切入点，针对提高钯基催化剂性能的关键科学问题，重点研究碱性纳米碳材料、钯、金属助剂协同催化醇醛一步氧化酯化的构效关系，研究调控纳米碳材料碱性的机制，建立碱性纳米碳材料高分散负载钯基双金属的方法，揭示助剂与钯之间的电荷转移规律，运用原位光谱检测反应中间体结构，通过量子化学计算模拟反应过渡态和速控步，阐明醇醛一步氧化酯化反应机理，获得反应过程的动力学模型，为高效、低负载量钯基催化剂的设计提供科学依据。本项目科学问题的提出源自于实践，相关研究成果服务于实践，非常具有针对性。本项目的成功实施将为高性能、低成本催化剂的设计、开发以及工业化推广提供重要的理论基础和实践指导。

中文关键词： 一步氧化酯化；甲基丙烯酸甲酯；N掺杂；碳材料；催化

英文摘要： Palladium is an important component of many catalysts and widely used in organic synthesis, fine chemical engineering and VOCs cleaning due to its excellent efficiency. However, palladium is one of the rare noble metals which made the cost of palladium-based catalysts high. In the commercial process of methyl methacrylate (MMA) produced by direct oxidative esterification of methylacrolein (MAL) with methanol, high cost of palladium-based catalysts is highlighted and becomes the restraining factor. Consequently, it is an urgent but pretty challenging task to develop much more efficient palladium-based catalysts with low Pd loadings. The project aims at the key issues of improving the efficiency of palladium-based catalysts, and we will emphasize the structure-function relationship of palladium-based catalysts. In details, the regularity of tuning the alkalinity of carbon nano material, the procedure of loading palladium-based bimetallic components onto alkaline carbon nano material, electron transfer between palladium and promoters, in-situ detection of intermediates, DFT calculation, the mechanism and the kinetic model of the direct oxidative esterification reaction will be investigated in this project. The above-mentioned investigations contribute to the development of efficient palladium-based catalysts with l

英文关键词： direct oxidative esterification；methyl methacrylate；N-doping；carbon material；catalysis