文献类型：期刊文献

英文题名：Mechanism-guided elaboration of ternary Au-Ti-Si sites to boost propylene oxide formation

作者：Wang, Gang[1];Du, Wei[1];Duan, Xuezhi[1];Cao, Yueqiang[1];Zhang, Zhihua[1];Xu, Jialun[1];Chen, Wenyao[1];Qian, Gang[1];Yuan, Weikang[1];Zhou, Xinggui[1];Chen, De[2]

机构：[1]East China Univ Sci & Technol, Sch Chem Engn, State Key Lab Chem Engn, Shanghai 200237, Peoples R China;[2]Norwegian Univ Sci & Technol, Dept Chem Engn, N-7491 Trondheim, Norway

年份：2021

卷号：1

期号：4

起止页码：885

外文期刊名：CHEM CATALYSIS

收录：WOS:【ESCI(收录号:WOS:000901289000014)】；

基金：This work was financially supported by the Natural Science Foundation of China (22038003 and 21922803), the Innovation Program of the Shanghai Municipal Education Commission (17ZR1407300), the Shanghai Rising-Star Program (17QA1401200), the Fundamental Research Funds for the Central Universities (222201718003), and the Open Project of the State Key Laboratory of Chemical Engineering (SKL-Che-15C03).

语种：英文

摘要：Mechanism-guided catalyst design and engineering at the scale of active sites has beendevelopedas apowerful tool for boostingcatalytic performance. Herein, we report an efficient selective silylation strategy for the elaborate fabrication of ternary Au-Ti-Si sites to boost propylene epoxidation with H-2 and O-2. Kinetics (isotopic) analysis, Fourier transforminfrared measurements, and theoretical calculations indicate an urgent necessity for selective consuming silanol sites not only to suppresspropyleneoxide (PO) ringopeningtobyproducts promoted by H-2 spillover but also to minimize PO inhibition effects. A continuous silylation treatment was developed to encourage the kinetically favorable formation of ternary Au-Ti(-OH)-Si(-O-SiR3) moiety. This delivers significantly improved H-2 efficiency of 42.5% in addition to the promising PO formation rate of 193 g h(-1) kgcat(-1) and PO selectivity of 95.7% with the long-term stability in excess of 200 h. These insights could pave the way for rationally fabricating catalyst active sites toward optimized performance.