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Surface coupling of methyl radicals for efficient low‐temperature oxidative coupling of methane

Chinese Journal of Catalysis 2021年第7期42卷 1117-1125页

作者： Shihui Zou Zhinian Li Qiuyue Zhou Yang Pan Wentao Yuan Lei He Shenliang Wang Wu Wen Juanjuan Liu Yong Wang Yonghua Du Jiuzhong Yang Liping Xiao Hisayoshi Kobayashi Jie Fan Key Laboratory of Applied Chemistry of Zhejiang Province Department of ChemistryZhejiang UniversityHangzhou 310036ZhejiangChina National Synchrotron Radiation Laboratory University of Science and Technology of ChinaHefei 230029AnhuiChina School of Materials Science and Engineering Zhejiang UniversityHangzhou 310027ZhejiangChina College of Materials&Environmental Engineering Hangzhou Dianzi UniversityHangzhou 310036ZhejiangChina National Synchrotron Light Source II Brookhaven National Laboratory Upton NY11973USA Emertus Professor of Kyoto Institute of Technology MatsugasakiSakyo‐kuKyoto 606‐8585Japan

Selective coupling of methyl radicals to produce C_(2) species(C2H4 and C2H6)is a key challenge for oxidative coupling of methane(OCM).In traditional OCM reaction systems,homogeneous transformation of methyl radicals in O_(2)‐containing gases are uncontrollable,resulting in limited C_(2) selectivity and ***,we demonstrate that methyl radicals generated by La_(2)O_(3)at low reaction temperature can selectively couple on the surface of 5 wt%Na2WO4/SiO_(2).The controllable surface coupling against overoxidation barely changes the activity of La_(2)O_(3)but boosts the C_(2)selectivity by three times and achieves a C_(2)yield as high as 10.9%at bed temperature of only 570℃.Structure‐property studies suggest that Na_(2)WO_(4) nanoclusters are the active sites for methyl radical *** strong CH_(3)·affinity of these sites can even endow some methane combustion catalysts with OCM *** findings of the surface coupling of methyl radicals open a new direction to develop OCM *** bifunctional OCM catalyst system,which composes of a methane activation center and a CH_(3)·coupling center,may deliver promising OCM performance at reaction temperatures below the ignition temperature of C2H6 and C2H4(~600℃)and is therefore more controllable,safer,and certainly more attractive as an actual process.

关键词： Oxidative coupling of methane Bifunctional catalysis methyl radicals Surface coupling La_(2)O_(3) Na_(2)WO_(4)/SiO_(2)

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