文献类型：期刊文献

英文题名：Trace Pd alloyed with Au to boost Au/uncalcined TS-1 catalyzed propane hydro-oxidation to acetone

作者：Sun, Jinwei[1];Zhang, Zhihua[1];Yang, Erchuan[1];Du, Wei[1];Liu, Fan[1];Xu, Kesheng[1];Zhong, Yuxia[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：17

期号：8

起止页码：7182

外文期刊名：NANO RESEARCH

收录：;EI(收录号：20242216188546);WOS:【SCI-EXPANDED(收录号:WOS:001232152300007)】；

基金：This work was financially supported by the Ministry of Science and Technology of the People's Republic of China under the Research Fund for National Key Research and Development Program of China (No. 2021YFA1501403), the National Natural Science Foundation of China (Nos. 22208093, 22038003, and 22178100), the Shanghai Science and Technology Innovation Action Plan (No. 22JC1403800), the Innovation Program of the Shanghai Municipal Education Commission, the Program of Shanghai Academic/Technology Research Leader (No. 21XD1421000), and the Fundamental Research Funds for the Central Universities. The authors would like to thank Yan Cui from Feringa Nobel Prize Scientist Joint Research Center of ECUST for HAADF-STEM measurement.

语种：英文

外文关键词：propane selective oxidation; acetone; hydrogen dissociation; Au-Pd alloy; synergy

摘要：Selective oxidation of propane to acetone (AC) with H2 and O2 provides a direct route to convert low-cost propane into value-added products. Unfortunately, the catalytic activity of conventional Au/Ti-based catalysts is constrained by the high energy barrier for H2 dissociation. Herein, uncalcined TS-1 supported Au-Pd bimetallic catalysts were prepared, and the relationship between the active-site structure and corresponding performance in the selective oxidation of propane with H2 and O2 in the gas phase was systematically investigated. In contrast to the liquid-phase reaction, trace Pd alloyed with Au triggered an increase in both catalytic activity and selectivity, in which Au20-Pd1/TS-1-B catalyst exhibited excellent activity (170 gACh-1kgcat-1) and AC selectivity (90.6%), much higher than those of the Au/TS-1-B catalyst (AC formation rate of 100 gACh-1kgcat-1 and AC selectivity of 86.3%). It was found that Pd was gradually isolated into monomers with the increase of Au/Pd molar ratio, and the synergy between Pd single atoms and Au improved the catalytic performance via enhancing hydrogen dissociation and modulating the electronic structure of Au. Furthermore, the reaction conditions were optimized based on the kinetics studies and the Au20-Pd1/TS-1-B catalyst exhibited enhanced H2 selectivity (45%) and long-term stability (over 130 h). The insights gained here can offer valuable guidance for the design of Au-Pd catalysts applicable to other gas-phase oxidation reactions.