甲醇选择氧化金属氧化物催化剂的结构与其催化性能的-物理化学学报.PDF

物理化学学报(Wuli Huaxue Xuebao) October Acta Phys. -Chim. Sin . 2012, 28 (10), 2315-2326 2315 [Review] doi: 10.3866/PKU.WHXB201209146 甲醇选择氧化金属氧化物催化剂的结构与其催化性能的关系 陈文龙 刘海超* (北京大学化学与分子工程学院, 绿色化学研究中心, 分子动态与稳态国家重点实验室, 北京分子科学国家实验室, 北京100871) 摘要: 甲醇是一个重要的平台分子, 实现其高效转化为能源和化学品的关键是揭示相关反应过程中催化剂的 结构与催化性能之间的关系和反应机理. 围绕这个关键问题, 以甲醇选择氧化为探针反应, 本文总结了负载氧 化钼、负载氧化钒和杂多酸等典型催化剂体系以及近年来发展的氧化铼、氧化钌等新催化剂体系在认识催化活 性中心结构和反应机理, 进而调控它们的氧化中心和酸中心等方面所取得的进展. 这些认识将有助于设计制备 性能优异的新催化剂和实现甲醇到目标氧化产物的定向转化. 关键词: 甲醇; 选择氧化; 氧化中心; 酸中心; 构效关系 中图分类号: O643 Relationship between the Structures of Metal Oxide Catalysts and Their Properties in Selective Oxidation of Methanol CHEN Wen-Long LIU Hai-Chao* (Beijing National Laboratory for Molecular Sciences, State Key Laboratory for Structural Chemistry of Unstable and Stable Species, Green Chemistry Center, College of Chemistry and Molecular Engineering, Peking University, Beijing 100871, P. R. China) Abstract: Methanol is an important platform molecule for the production of energy and chemicals. For its efficient utilization, it is of critical significance to clarify the relationship between the structures of the catalysts and their performance as well as the corresponding reaction mechanisms. In this review, we summarized some recent progress in the understanding of the active structures of several metal oxide-based catalysts and the reaction mechanism, and the consequent tuning of their redox and acid sites for the sel