文献类型：期刊文献

英文题名：Identifying the Activity Origin of a Single-Atom Au1/Nb2O5 Catalyst for Hydrodeoxygenation of Methylcatechol: A Stable Substitutional Au+ Site

作者：Xia, Jie[1]; Dong, Lin[1,2]; Liu, Xiaohui[1]; Chernikov, Roman[3]; Shakouri, Mohsen[3]; Hu, Yongfeng[3]; Guo, Yong[1]; Wang, Jianjian[4]; Song, Kepeng[5]; Hu, Peijun[1,6]; Wang, Yanqin[1]; Wang, Haifeng[1]

机构：[1] Key Laboratory for Advanced Materials and Joint International Research Laboratory of Precision Chemistry and Molecular Engineering, Feringa Nobel Prize Scientist Joint Research Center, Research Institute of Industrial Catalysis and Centre for Computational Chemistry, School of Chemistry and Molecular Engineering, East China University of Science and Technology, Shanghai, 200237, China; [2] Jiangsu Co-Innovation Center of Efficient Processing and Utilization of Forest Resources, International Innovation Center for Forest Chemicals and Materials, Jiangsu Province Key Laboratory of Green Biomass-Based Fuels and Chemicals, College of Chemical Engineering, Nanjing Forestry University, Nanjing, 210037, China; [3] Canadian Light Source Inc., 44 Innovation Boulevard, Saskatoon, SK, S7N 2V3, Canada; [4] Multi-Scale Porous Materials Center, Institute of Advanced Interdisciplinary Studies, Chongqing University, Chongqing, 400044, China; [5] Advanced Membranes and Porous Materials Center, Physical Science and Engineering Division, King Abdullah University of Science and Technology, Thuwal, 23966-6900, Saudi Arabia; [6] School of Chemistry and Chemical Engineering, The Queen’s University of Belfast, Belfast, BT9 5AG, United Kingdom

年份：2023

卷号：13

期号：9

起止页码：6093

外文期刊名：ACS Catalysis

收录：EI(收录号：20231814042818)

语种：英文

外文关键词：Atoms - Catalyst activity - Density functional theory - Design for testability - Lattice theory - Molecular oxygen

摘要：Developing effective and stable single-atom catalysts (SACs) is a significant but challenging task, which requires the identification of single-atom metal sites and their configurations. Herein, we report a single-atom Au1/Nb2O5 catalyst for the hydrodeoxygenation of methylcatechol, a lignin model compound, which maintains stability in five consecutive conversions. Combined with the density functional theory (DFT) calculations, the Au+ located at the Nb lattice site with two concomitant oxygen vacancies (Au@Nbv-2Ov) is identified as the thermodynamically favorable Au single-atom species and dominates the activity for molecular H2 dissociation via a heterolytic mechanism. Moreover, the presence of oxygen vacancies in Au@Nbv-2Ov facilitates the adsorption of methylcatechol, resulting in efficient cleavage of C-O bonds. Consequently, we design a catalyst with more Au+ sites, which exhibits enhanced catalytic activity. This work systematically elucidates the structure-activity relationship and provides a promising strategy to optimize SACs for the hydrodeoxygenation reaction. ? 2023 American Chemical Society.