文献类型：期刊文献

英文题名：Mechanistic insights into the atmosphere-dependent strong metal-support interactions of Au/ZnO catalysts for oxidative esterification

作者：Xie, Yongkai[1];Zhang, Zhongyao[1];Zhang, Xiangxue[1];Chen, Wenyao[1];Chen, De[1,2];Zhou, Xinggui[1];Duan, Xuezhi[1]

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

年份：2026

卷号：330

外文期刊名：CHEMICAL ENGINEERING SCIENCE

收录：;EI(收录号：20261420420577);WOS:【SCI-EXPANDED(收录号:WOS:001733956700001)】；

基金：Funding sources: This work was financially supported by the National Key R&D Program of China (2024YFA1510303) , the Natural Science Foundation of China (22478107, 22038003, 22178100,

语种：英文

外文关键词：Strong metal-support interactions; Oxygen vacancy; Methyl methacrylate; Active site; Au catalyst

摘要：Strong metal-support interactions (SMSI) are pivotal for constructing interfacial active sites, yet its precise regulation remains a formidable challenge. Here, we report a facile strategy to modulate the atmosphere-dependent SMSI in Au/ZnO catalysts by strictly regulating the oxygen partial pressure during thermal treatment. We reveal that the encapsulation degree of Au particles exhibits a volcano-shaped dependence on oxygen partial pressure, which drives electron transfer from Au to the support to create abundant interfacial oxygen vacancies (Au-OV-Zn). For the oxidative esterification of methacrolein, mechanistic investigations reveal that these interfacial defects constitute frustrated Lewis acid-base pairs to promote the formation of hemiacetal intermediates, and simultaneously serve as active sites for oxygen activation. The activated lattice oxygen migrates to the Au surface and generate active Au-O species that effectively overcome the kinetic barrier of the rate-determining beta-H elimination. Driven by this interfacial synergy, the catalyst exhibiting the most pronounced SMSI achieves state-of-the-art performance with an MMA yield of 91.8%. These findings provide a new strategy for the design of high-performance catalysts via interfacial defect engineering.