Liu Lichen, Ge Chengyan, Zou Weixin, Gu Xianrui, Gao Fei, Dong Lin
Key Laboratory of Mesoscopic Chemistry of Ministry of Education, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing 210093, P. R. China.
Phys Chem Chem Phys. 2015 Feb 21;17(7):5133-40. doi: 10.1039/c4cp05449k.
Metal-support interactions between Au and TiO2 are studied based on Au/TiO2 catalysts with different TiO2 crystal planes exposed. With ex situ XPS, TEM and in situ DRIFTS, we have investigated the crystal-plane-dependent metal-support interaction effects on the physiochemical properties of Au/TiO2 catalysts. Based on the structural characterization and spectroscopic results, we can observe chemical oscillations (including the electronic structures of Au nanoparticles and the interaction between Au/TiO2 catalysts and CO molecules) during alternate H2 and O2 pre-treatments. Their variation tendencies of oscillations are greatly dependent on the crystal planes of TiO2 and the pre-treatment temperature. Furthermore, their surface and electronic changes after H2 and O2 pre-treatments can be well correlated with their catalytic activities in CO oxidation. Electron-transfer processes across the Au-TiO2 interface are proved to be the origin accounting for their changes after H2 and O2 pre-treatments. The different electronic structures of different TiO2 crystal planes should have relationships with the crystal-plane-dependent metal-support interaction effects in Au/TiO2.
基于暴露不同TiO₂晶面的Au/TiO₂催化剂,研究了Au与TiO₂之间的金属-载体相互作用。通过非原位XPS、TEM和原位DRIFTS,我们研究了晶面依赖性金属-载体相互作用对Au/TiO₂催化剂物理化学性质的影响。基于结构表征和光谱结果,我们可以观察到在交替进行H₂和O₂预处理期间的化学振荡(包括Au纳米颗粒的电子结构以及Au/TiO₂催化剂与CO分子之间的相互作用)。其振荡的变化趋势很大程度上取决于TiO₂的晶面和预处理温度。此外,H₂和O₂预处理后的表面和电子变化与它们在CO氧化中的催化活性密切相关。跨Au-TiO₂界面的电子转移过程被证明是其在H₂和O₂预处理后发生变化的原因。不同TiO₂晶面的不同电子结构应与Au/TiO₂中晶面依赖性金属-载体相互作用效应有关。