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内蒙古自治区呼和浩特市赛罕区大学西街235号 邮编: 010021
作者机构:Key Laboratory of Optoelectronic Materials Chemistry and Physics Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences Fuzhou Fujian 350002 China Key Laboratory of Design & Assembly of Functional Nanostructures Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences Fuzhou Fujian 350002 China Fujian Science & Technology Innovation Laboratory for Optoelectronic Information of China Fuzhou Fujian 350108 China Advanced Energy Science and Technology Guangdong Laboratory 29 Sanxin North Road Huizhou Guangdong 116023 China
出 版 物:《Angewandte Chemie》 (应用化学)
年 卷 期:2022年第134卷第32期
页 面:e202207211-e202207211页
学科分类:081704[工学-应用化学] 08[工学] 0817[工学-化学工程与技术]
主 题:Carbon Dioxide Ceria Interfaces Methane Porosity
摘 要:Catalytic conversion of CH 4 to C 2 H 4 plays an important role in the light olefin industry. Here, we report the electrochemical conversion of CH 4 to C 2 H 4 /C 2 H 6 at the anode with the electrolysis of CO 2 to CO at the cathode in a solid oxide electrolyser. We constructed well-defined interfaces that function as three-phase boundaries by exsolving single-crystalline Ni nanoparticles in porous single-crystalline CeO 2 monoliths. We engineered the chemical states and flux of active oxygen species for the oxidation of CH 4 at the anode by controlling voltage and temperature. We show the unprecedented C 2 selectivity (C 2 H 4 and C 2 H 6 ) of ≥99.5 % at a CH 4 conversion of ≈7 %. The electrolyser exhibits excellent durability without performance degradation being observed in a continuous operation of 100 hours. Our work enables a novel path for the selective conversion of CH 4 /CO 2 into useful chemicals, and the technique of building well-defined interfaces may find potential applications in other fields.