Measurements of surface reaction rates and design of active surfaces

本研究的目的是建立一种测量表面反应速率的方法，并建立设计高性能新型催化剂的策略。在电子刺激脱附系统中安装了脉冲分子束剂量计和氮气激光器。利用TAP系统研究了以二氧化硅为载体制备的用于沼气制取合成气反应的镍催化剂。对于设计新颖的催化剂表面，实现了离子液体分子在二氧化硅载体表面的固定化和与金属氯酸盐阴离子的成盐。实现了钴氧化物和氢氧化物纳米晶的形状控制。用密度泛函理论方法计算了硅胶表面Ru单核络合物和HZSM-5骨架Re簇合物催化剂的催化活性结构，并阐明了反应机理。

The purpose of this research was to establish a method for measuring surface reaction rates as well as to establish a strategy for designing novel catalysts with high performances. Pulse molecular beam dosers and nitrogen Laser were installed in the Electron Stimulated Desorption system. TAP system was used to study a Ni catalyst prepared on silica support for reactions from biogas to syngas. For novel designed catalyst surfaces, immobilization of ionic liquid molecules on silica support surfaces and salt formation with chlorometallate anions were achieved. Shape control of nanocrystals of cobalt oxides and hydroxides were achieved. Density Functional Theory calculations were performed to obtain active structures of catalytic reactions and to clarify reaction mechanism for a Ru mononuclear complex attached on silica surface and Re cluster catalysts prepared in HZSM-5 framework.