文献类型：期刊文献

英文题名：ZSM-5-confined Cr1-O4 active sites boost methane direct oxidation to C1 oxygenates under mild conditions

作者：Zeng, Mengyu[1,2];Cheng, Lu[3,4,5,6];Gu, Qingqing[7];Yang, Bing[7];Yu, Baiyang[1,2];Xu, Jing[8];Zhang, Ying[1,2];Pan, Chengsi[1,2];Cao, Xiao-Ming[3,4,5,6];Lou, Yang[1,2];Zhu, Yongfa[9]

机构：[1]Jiangnan Univ, Sch Chem & Mat Engn, Key Lab Synthet & Biol Colloids, Minist Educ, Wuxi 214122, Jiangsu, Peoples R China;[2]Jiangnan Univ, Int Joint Res Ctr Photorespons Mol & Mat, Wuxi 214122, Jiangsu, Peoples R China;[3]East China Univ Sci & Technol, Key Lab Adv Mat, Shanghai 200237, Peoples R China;[4]East China Univ Sci & Technol, Feringa Nobel Prize Scientist Joint Res Ctr, Sch Chem & Mol Engn, Shanghai 200237, Peoples R China;[5]East China Univ Sci & Technol, Ctr Computat Chem, Shanghai 200237, Peoples R China;[6]East China Univ Sci & Technol, Res Inst Ind Catalysis, Shanghai 200237, Peoples R China;[7]Dalian Inst Chem Phys, Dalian Natl Lab Clean Energy, 457 Zhongshan Rd, Dalian 116023, Peoples R China;[8]Jiangnan Univ, Sch Food Sci & Technol, Wuxi 214122, Jiangsu, Peoples R China;[9]Tsinghua Univ, Dept Chem, Beijing 100084, Peoples R China

年份：2023

卷号：1

期号：2

起止页码：153

外文期刊名：EES CATALYSIS

收录：WOS:【ESCI(收录号:WOS:001362414100001)】；

基金：This project was supported financially by the National Key R&D Program of China (2021YFB3501900), the National Natural Science Foundation of China (21908079, U21A20326, 21872145, 21902009, 22172065, 22022302, 92045303 and 91845111), the Jiangsu Specially-Appointed Professor (1046010241211400), the Natural Science Foundation of Jiangsu Province (BK20211239, BK20201345, BK20221541), the State Key Laboratory of Fine Chemicals, the Dalian University of Technology (KF2005). We also thank the Central Laboratory, School of Chemical and Material Engineering, Jiangnan University.

语种：英文

摘要：Direct oxidation of methane (DOM) to value-added chemicals is of great significance but is still challenging under mild conditions. Herein, we report that Cr1-O4 as an active site in a ZSM-5 anchored Cr single atom catalyst (Cr1/ZSM-5 SAC) can efficiently catalyse the DOM to form value-added C1 oxygenated products with a productivity of 21 100 mu mol gcat-1 h-1 and a selectivity of 99.8% at 50 degrees C within 30 min, which outperforms most reported state-of-the-art catalysts. Density functional theory (DFT) calculations and experimental results show that Cr1 atoms anchored on the wall of ZSM-5 micropores form the Cr1-O4 active sites, which boosts the formation of the reactive oxygen species (adsorbed OH species) and the activation of a C-H bond in CH4. We believe that our atomic-level design strategy on a non-noble metal offers an approach to rationally design efficient catalysts for methane conversion.