Kinetics and mechanism of propylene hydro-oxidation to acrolein on Au catalysts  

作　　者：Wei Du Zhihua Zhang Nan Song Xuezhi Duan Xinggui Zhou 

机构地区：[1]State Key Laboratory of Chemical Engineering,School of Chemical Engineering,East China University of Science and Technology,Shanghai 200237,China

出　　处：《Nano Research》2024年第1期354-363,共10页纳米研究（英文版）

基　　金：financially supported by the Research Fund for National Key R&D Program of China(No.2021YFA1501403);the National Natural Science Foundation of China(Nos.22038003,21922803,22178100,and 22208094);the Program of Shanghai Academic/Technology Research Leader(No.21XD1421000);the Shanghai Science and Technology Innovation Action Plan(No.22JC1403800);the Innovation Program of the Shanghai Municipal Education Commission.

摘　　要：Propylene epoxidation by H_(2)and O_(2)to propylene oxide(PO)over the Au-Ti bifunctional catalysts,as an ideal reaction for PO production,has attracted great interest.Revealing the mechanism of acrolein formation is of great importance for understanding the mechanism of molecular oxygen activation and the formation of hydroperoxo species on the Au sites.Here,we investigate the reaction mechanism of propylene oxidation to acrolein on the Au/uncalcined TS-1(Au/TS-1-B)catalyst through a combination of multiple characterization,H_(2)/D_(2)exchange,kinetics experiment,and modeling.The Ti sites are found to be non-essential to acrolein formation.Moreover,the acrolein formation on the Au/TS-1-B catalyst is confirmed to be promoted by H_(2)through hydroperoxo species formation,which includes two main steps:propylene dehydrogenation to*C_(3)H_(5)with the aid of*OOH species,and*C_(3)H_(5)oxidation by*OOH to acrolein.The latter step is determined to be the rate-determining step because the corresponding kinetics model gives the best description for experimental results.This work not only provides kinetics insights for the propylene hydro-oxidation to acrolein on the Au-Ti bifunctional catalysts,but also facilitates the rational design of Au catalysts with high activity and selectivity in the direct propylene epoxidation with H_(2)and O_(2).

关 键 词：KINETICS mechanism GOLD ACROLEIN hydro-oxidation 

分 类 号：O64[理学—物理化学]