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，以及建立一种设计具有高性能的新型催化剂的策略。在电子刺激脱附系统中安装了脉冲分子束剂量器和氮激光器。采用TAP体系对以二氧化硅为载体制备的Ni催化剂进行了生物气制合成气反应研究。对于新设计的催化剂表面，实现了离子液体分子在二氧化硅载体表面上的固定化和与氯金属酸盐阴离子的成盐。实现了钴氧化物和氢氧化物纳米晶体的形状控制。采用密度泛函理论计算了负载于SiO2表面的Ru单核配合物和负载于HZSM-5骨架上的Re簇催化剂的催化反应活性结构，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.