Visible-light driven room-temperature coupling of methane to ethane by atomically dispersed Au on WO_(3)  

作　　者：Xing Yang Wu Zhiyuan Tang Xiaoxu Zhao Xin Luo Stephen John Pennycook Song Ling Wang 

机构地区：[1]China-UK Low Carbon College,Shanghai Jiao Tong University,Shanghai 201306,China [2]School of Environmental Science and Engineering,Shanghai Jiao Tong University,Shanghai 200240,China [3]State Key Laboratory of Optoelectronic Materials and Technologies,Centre for Physical Mechanics and Biophysics,School of Physics,Sun Yat-sen University,Guangzhou 510275,Guangdong,China [4]Institute Department of Materials Science and Engineering,National University of Singapore,Singapore 117575,Singapore [5]Shanghai Institute of Pollution Control and Ecological Security,Shanghai 200092,China

出　　处：《Journal of Energy Chemistry》2021年第10期195-202,I0006,共9页能源化学（英文版）

基　　金：sponsored by Shanghai Pujiang Program(No.19PJ1405200);the Startup Fund for Youngman Research at SJTU(SFYR at SJTU,No.WF220516003)。

摘　　要：Gold(Au)as co-catalyst is remarkable for activating methane(CH4),especially atomically dispersed Au with maximized exposing active sites and specific electronic structure.Furthermore,singlet oxygen(^(1)O_(2))typically manifests a mild redox capacity with a high selectivity to attack organic substrates.Peroxomonosulfate(PMS)favors to produce oxidative species 102 during the photocatalytic reactions.Thus,combining atomic Au as co-catalyst and ^(1)O_(2) as oxidant is an effective strategy to selectively convert CH4.Herein,we synthesized atomically dispersed Au on WO_(3)(Au/WO_(3)),where Au was in the forms of single atoms and clusters.At room temperature,such Au/WO_(3) exhibited enhanced photocata lytic conversion of CH4 to CH3 CH3 with a selectivity,up to 94%,under visible light.The radicals-pathway mechanism of CH4 coupling has also been investigated through detection and trapping experiment of active species.Theoretical calculations further interpret the electronic structure of Au/WO_(3) and tip-enhanced local electric field at the Au sites for promoting CH4 conversion.

关 键 词：PHOTOCATALYSIS Single-atom Au METHANE ETHANE Visible light 

分 类 号：X701[环境科学与工程—环境工程] O643.32[理学—物理化学] O644.1[理学—化学]