文献类型：期刊文献

英文题名：Surface Engineering and Kinetics Behaviors of Au/Uncalcined TS-1 Catalysts for Propylene Epoxidation with H2 and O2

作者：Wang, Gang[1];Cao, Yueqiang[1];Zhang, Zhihua[1];Xu, Jialun[1];Lu, Mengke[1];Qian, Gang[1];Duan, Xuezhi[1];Yuan, Weikang[1];Zhou, Xinggui[1]

机构：[1]East China Univ Sci & Technol, State Key Lab Chem Engn, Shanghai 200237, Peoples R China

年份：2019

卷号：58

期号：37

起止页码：17300

外文期刊名：INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH

收录：;EI(收录号：20194107511628);WOS:【SCI-EXPANDED(收录号:WOS:000487179800018)】；

基金：This work was financially supported by the Natural Science Foundation of China (21922803 and 91434117), the Natural Science Foundation of Shanghai (17ZR1407300), the Shanghai Rising-Star Program (17QA1401200), the Fundamental Research Funds for the Central Universities (222201718003), and the Open Project of State Key Laboratory of Chemical Engineering (SKL-Che-15C03).

语种：英文

外文关键词：Activation energy - High resolution transmission electron microscopy - Propylene - Thermogravimetric analysis - Activation analysis - Catalyst activity - X ray photoelectron spectroscopy - Scanning electron microscopy - Reaction kinetics - Catalyst selectivity - Surface properties

摘要：Uncalcined TS-1-immobilized Au bifunctional catalysts have been demonstrated to be highly active yet stable for the propylene epoxidation with H-2 and O-2. The objective of this study is to further engineer the surface properties of uncalcined TS-1 toward enhanced bifunctional catalysis. A strategy by increasing the reduction temperature is proposed to remove the residual TPA(+) template on the external surfaces, and the resultant Au/TS-1-B-300 catalyst gives rise to simultaneously enhanced activity, propylene oxide (PO) selectivity, and H-2 efficiency. These phenomena are explained by more exposed Ti-active sites and targeted catalysts' electronic properties based on high-angle annular dark-field scanning transmission electron microscopy, thermal gravimetric analysis, UV-vis, Fourier transform infrared spectra, and X-ray photoelectron spectroscopy measurements. Furthermore, kinetics analysis demonstrates a much lower activation energy for the main reaction to form PO, suggesting the existence of an appropriate reaction temperature for the PO yield. The obtained insights could shed new light on rationally designing and optimizing the catalysts by engineering the surface properties.