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 plus Site

作者：Xia, Jie[1,2,3];Dong, Lin[1,2,3,4];Liu, Xiaohui[1,2,3];Chernikov, Roman[5];Shakouri, Mohsen[5];Hu, Yongfeng[5];Guo, Yong[1,2,3];Wang, Jianjian[6];Song, Kepeng[7];Hu, Peijun[1,2,3,8];Wang, Yanqin[1,2,3];Wang, Haifeng[1,2,3]

机构：[1]East China Univ Sci & Technol, Key Lab Adv Mat, Shanghai 200237, Peoples R China;[2]East China Univ Sci & Technol, Res Inst Ind Catalysis, Feringa Nobel Prize Scientist Joint Res Ctr, Joint Int Res Lab Precis Chem & Mol Engn, Shanghai 200237, Peoples R China;[3]East China Univ Sci & Technol, Ctr Computat Chem, Sch Chem & Mol Engn, Shanghai 200237, Peoples R China;[4]Nanjing Forestry Univ, Coll Chem Engn, Int Innovat Ctr Forest Chem & Mat, Jiangsu Prov Key Lab Green Biomass Based Fuels & C, Nanjing 210037, Peoples R China;[5]Canadian Light Source Inc, Saskatoon, SK S7N 2V3, Canada;[6]Chongqing Univ, Inst Adv Interdisciplinary Studies, Multiscale Porous Mat Ctr, Chongqing 400044, Peoples R China;[7]King Abdullah Univ Sci & Technol, Adv Membranes & Porous Mat Ctr, Phys Sci & Engn Div, Thuwal 239666900, Saudi Arabia;[8]Queens Univ Belfast, Sch Chem & Chem Engn, Belfast BT9 5AG, North Ireland

年份：2023

卷号：13

期号：9

起止页码：6093

外文期刊名：ACS CATALYSIS

收录：;WOS:【SCI-EXPANDED(收录号:WOS:000974040000001)】；

基金：? ACKNOWLEDGMENTS This project was supported financially by the National Key R&D Program of China (2021YFA1500700 and 2022YFA1504903) , the National Natural Science Foundation of China (21832002, 21872050, 22002043, and 22102056) , Shanghai Municipal Science and Technology Major Project (2018SHZDZX03) , and the Programme of Introducing Talents of Discipline to Universities (B16017) .

语种：英文

外文关键词：single-atom catalyst; Au-based catalyst; activity site; hydrodeoxygenation

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.