文献类型：期刊文献

英文题名：Kinetic insights into reaction pathways of acrolein formation in propylene epoxidation by H 2 and O 2 over Au/TS-1 catalyst

作者：Du, Wei[1];Zhang, Zhihua[1];Wang, Jundi[1];Song, Nan[1];Duan, Xuezhi[1];Zhou, Xinggui[1]

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

年份：2024

卷号：487

外文期刊名：CHEMICAL ENGINEERING JOURNAL

收录：;EI(收录号：20241415840103);WOS:【SCI-EXPANDED(收录号:WOS:001218140800001)】；

基金：This work was supported by the Ministry of Science and Technology of the People's Republic of China under the Research Fund for National Key R & D Program of China (2021YFA1501403) , the National Natural Science Foundation of China (22038003, 22208093, 22178100, 21922803) , the Program of Shanghai Academic/Technology Research Leader (21XD1421000) , the Shanghai Science and Technology Innovation Action Plan (22JC1403800) , and the Innovation Program of the Shanghai Municipal Education Commission.

语种：英文

外文关键词：Kinetics; Acrolein; TS-1; Gold; Propylene oxide

摘要：Propylene epoxidation by H 2 and O 2 to propylene oxide (HOPO), as a novel method for PO production, has attracted widespread attention due to its economic and environmental advantages. Acrolein is a notable byproduct arising in HOPO reaction over Au/TS-1 catalyst, and is traditionally thought to be exclusively formed on Au site through propylene oxidation. However, on the intraporous and external surface Au sites of Au -Ti catalysts, the HOPO reaction have been shown to proceed by different mechanisms, yet the effect of active sites distribution on acrolein formation is far from being understood. Herein, we found that the reaction orders in acrolein formation on Au/TS-1 catalyst (H 2 , 0.19; O 2 , 0.44; C 3 H 6 , 0.44) relative to Au/TS-1 with blocked pores (Au/TS-1-B) catalyst (H 2 , -0.36; O 2 , 0.61; C 3 H 6 , 0.52) were quite different, suggesting a variation in the reaction pathway on the catalysts with different Au locations. Moreover, it is found that PO can be converted to acrolein by O 2 on TS -1 zeolite, which is absent on TS -1-B zeolite without micropores. Consequently, acrolein formation on Au/TS-1 catalyst can proceed through two parallel pathways: propylene hydro -oxidation on Au site, and PO conversion by O 2 inside micropores. Furthermore, by designing and preparing the Au/TS-1 catalysts with different structures, the Au locations are closely related to acrolein formation mechanism and kinetic behaviors. This work provides kinetic insights into the acrolein formation pathways in the HOPO reaction on Au/TS-1 catalyst, and is helpful to the rational design and preparation of efficient catalysts with high selectivity.