文献类型：期刊文献

英文题名：Interface-enhanced catalytic performance of TiO2-supported Cu and Au for dimethyl oxalate hydrogenation: A comparative microkinetic analysis

作者：Jing, Li-Jun[1];Yan, Wei-Qi[1];Xiao, Han-Jie[1];Lei, Ming[1];Cao, Yue-Qiang[1];Sui, Zhi-Jun[1];Zhou, Jing-Hong[1];Zhou, Xing-Gui[1];Chen, De[2];Zhu, Yi-An[1]

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

年份：2023

卷号：281

外文期刊名：CHEMICAL ENGINEERING SCIENCE

收录：;EI(收录号：20233514638108);WOS:【SCI-EXPANDED(收录号:WOS:001068253000001)】；

基金：This work is supported by the National Natural Science Foundation of China (22073027, 91645122, and 22178102) . The computational time provided by the Notur project is highly acknowledged.

语种：英文

外文关键词：Density functional theory; Metal-oxide interface; DMO hydrogenation; Oxygen vacancies; Microkinetic analysis

摘要：The electronic structures of Cu-TiO2 and Au-TiO2 and their catalytic behaviors in the hydrogenation of dimethyl oxalate (DMO) have been studied by the stochastic surface walking-global neural network potential method, density functional theory calculation, and microkinetic analysis. Calculated results indicate that metal clusters on the pristine and oxygen-deficient TiO2 are mostly coordinated to O2c ions, and the defective surface may provide additional oxygen vacancies for Cu6 and Au6 cluster anchoring. It turns out that the interfacial Ti5c and Cu & delta;+/ Au & delta;-ions provide adsorption and hydrogenation sites for the reaction intermediates with unsaturated O and C atoms, respectively. The turnover frequency for DMO consumption is much higher on Cu-TiO2 than on Au-TiO2, Cu(1 1 1), and Cu(2 1 1) at 443.15 K and 20 bar of total pressure. Given the satisfactory methyl glycolate (MG) selectivity, the Cu-TiO2 catalyst has the potential to act as an excellent catalyst for the selective MG production.