文献类型：期刊文献

英文题名：Direct oxidation of methane to oxygenates on supported single Cu atom catalyst

作者：Tang, Xuan[1,2];Wang, Li[1];Yang, Bing[3];Fei, Chen[1];Yao, Tingyi[2];Liu, Wei[3];Lou, Yang[2];Dai, Qiguang[1];Cai, Yafeng[1];Cao, Xiao-Ming[1];Zhan, Wangcheng[1];Guo, Yanglong[1];Gong, Xue-Qing[1];Guo, Yun[1]

机构：[1]East China Univ Sci & Technol, Res Inst Ind Catalysis, Sch Chem & Mol Engn, 130 Meilong Rd, Shanghai 200237, Peoples R China;[2]Jiangnan Univ, Sch Chem & Mat Engn, Int Joint Res Ctr Photorespons Mol & Mat, Key Lab Synthet & Biol Colloids, Wuxi 214122, Jiangsu, Peoples R China;[3]Dalian Inst Chem Phys, Dalian Natl Lab Clean Energy, 457 Zhongshan Rd, Dalian 116023, Peoples R China

年份：2021

卷号：285

外文期刊名：APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY

收录：;EI(收录号：20210309776102);WOS:【SCI-EXPANDED(收录号:WOS:000623242700002)】；

基金：This project was supported financially by the National Key Research and Development Program of China (2016YFC0204300 and 2018YFA0208600), the National Natural Science Foundation of China (21908079, 21571061, 91845111, 21673072, 22022302, 21872145), the Startup Funding at Jiangnan University (1045210322190170) and the State Key Laboratory of Fine Chemicals, Dalian University of Technology (KF2005). The authors gratefully thank the staff at the BL14W1 beamline at the Shanghai Synchrotron Radiation Facility (SSRF), and the Research Center of Analysis and Test at East China University of Science and Technology for help on data and characterization. The authors appreciate the valuable suggestions from Prof. Yongfa Zhu (Tsinghua University).

语种：英文

外文关键词：Methane direct conversion; Single Cu atoms; Preferential methane activation

摘要：Catalytically converting CH4 to chemicals and fuels is of paramount importance but remains a major challenge to simultaneously obtain high activity and selectivity. Here, we report Cu-1/ZSM-5 single atom catalyst is highly active (C1 oxygenates productivity of 4800 mu mol.g(cat)(-1) at 50 degrees C and 12,000 mu mol.g(cat)(-1) at 70 degrees C within 30 min) and selective (C1 oxygenates selectivity of 99 % at 50 degrees C) for direct CH4 oxidation, comparable to most of those state-of-the-art noble metal catalysts. The combined DFT calculation, electronic microscope, X-ray absorption and electron paramagnetic resonance results confirm that each isolated Cu atom stabilized by four O moieties on the ZSM-5 support possesses uniform Cu-1-O-4 entity as active site and preferentially activates CH4 instead of CH3OH that is advantageous for highly selective C1 oxygenates production, especially for methanol. Our molecular-level finding on the atomic structure of Cu active site paves the way to design better catalysts for methane conversion.