铑、铜-基催化剂上CO临氢转化的模型催化研究

CO hydrogenation to the low molecular weight alcohols, alkenes, gasoline and diesel by Fischer-Tropsch reaction, is the key catalytic processes for optimal utilization of non oilbased fossil resources. Strong metal-support interaction (SMSI) has been found to promote the CO hydrogenation performance significantly. In the present project, various model surfaces that mimic SMSI, like MnOx/Rh(111), MnOx/Rh(100), FeOx/Rh(111), SiO2/Cu(111), SiO2/Cu(100), etc. will be synthesized under ultra-high vacuum (UHV). CO hydrogenation performance on these model surfaces will be measured in the home-built model catalysis reaction cell. The surface structures, the surface active species, physical chemistry properties, and the changes of these model surfaces will be characterized under catalytic conditions by wide spectral range in-situ infrared reflection adsorption spectroscopy (IRAS), ambient pressure X-ray photoemission spectroscopy (APXPS) and ultra-violet photoemission spectroscopy (UPS). Detail correlation between the surface structure and catalytic performance can be established. Furthermore, using these model surfaces, by combining with modern surface science techniques, the nature of the catalytically active sites, mechanism of catalysis, the key aspects that controlled the selectivity, as well as the promotion effects of SMSI, can be better understood.

CO 加氢制低碳醇、低碳烯烃和经费托合成制汽、柴油等是非油基碳资源优化利用的重要催化反应，据报道金属－氧化物载体强相互作用(SMSI)对 CO 加氢性能有显著促进作用。本项目拟在前期工作基础上，在超高真空环境下研制MnOx/Rh(111), MnOx/Rh(100), FeOx/Rh(111), SiO2/Cu(111), SiO2/Cu(100)等模拟SMSI的模型催化剂表面，应用具备宽波段原位镜面反射红外吸收光谱的模型催化反应装置测定其CO加氢相关反应的催化性能和反应过程中的表面物种，结合新购建的近常压X-光电子能谱(APXPS)和紫外光电子能谱(UPS)测定实际催化反应条件下SMSI模型催化剂表面的动态变化、表面结构等，建立催化剂的结构～性能的关系，并进而研究其活性位的本质、反应机理、影响CO临氢反应选择性的关键控制因素、以及SMSI作用机制的本质。

CO 加氢制低碳醇、低碳烯烃和经费托合成制汽、柴油等是非油基碳资源优化利用的重要催化反应，据报道金属－氧化物载体强相互作用(SMSI)对 CO 加氢性能有显著促进作用。本项目在超高真空环境下、不同蒸着条件、氧气分压、氧化/退火温度成功研制MnOx/Rh(111), FeOx/Rh(111), MnOx/Ni(111), SiO2/Cu(111), SiO2/Cu(110), TiOx/Cu(111), TiOx/Cu(110)等模拟SMSI的具不同结构的模型催化剂表面，应用AES, LEED, HREELS, XPS, LEIS, STM, IRAS, APXPS和UPS等表征了这些模型表面的生长模式、表面原子结构和电子结构，测试了模型表面上CO氧化/加氢、烯烃/炔烃加氢等反应的催化性能，考察在接近实际催化反应条件下表界面的动态变化、表面吸附物种，关联构效关系。并开展了几个实际催化剂体系的金属-氧化物作用研究。