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.
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 selective oxidation of methanol.The catalysts included supported molybdenum oxides,supported vanadium oxides,and heteropolyacids with Keggin structures as well as rhenium oxides and ruthenium oxides recently explored for the methanol oxidation.Such progress provides insights into the design of novel catalysts more efficient for the oxidative conversion of methanol towards the targeted products.