Interfacial Enhancement by γ-Al2O3 of Electrochemical Oxidative Dehydrogenation of Ethane to Ethylene in Solid Oxide Electrolysis Cells

被引:36
作者
Song, Yuefeng [1 ,2 ]
Lin, Le [1 ,3 ]
Feng, Weicheng [1 ,2 ]
Zhang, Xiaomin [1 ]
Dong, Qiao [2 ,4 ]
Li, Xiaobao [2 ,4 ]
Lv, Houfu [1 ,2 ]
Liu, Qingxue [1 ,2 ]
Yang, Fan [1 ]
Liu, Zhi [3 ,4 ]
Wang, Guoxiong [1 ]
Bao, Xinhe [1 ]
机构
[1] Chinese Acad Sci, CAS Ctr Excellence Nanosci, Dalian Inst Chem Phys, State Key Lab Catalysis, Zhongshan Rd 457, Dalian 116023, Peoples R China
[2] Univ Chinese Acad Sci, Beijing 100039, Peoples R China
[3] ShanghaiTech Univ, Sch Phys Sci & Technol, Shanghai 200031, Peoples R China
[4] Chinese Acad Sci, Shanghai Inst Microsyst & Informat Technol, State Key Lab Funct Mat Informat, Shanghai 200050, Peoples R China
基金
国家重点研发计划; 中国国家自然科学基金;
关键词
ethane; gamma-aluminum oxide; interfaces; oxidative dehydrogenation; solid oxide electrolysis cell; GAMMA-ALUMINA; COMPOSITE CATHODES; CATALYTIC-ACTIVITY; PERFORMANCE; OXYGEN; ELECTRODES; STABILITY; HYDROGEN; BEHAVIOR; METALS;
D O I
10.1002/anie.201908388
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Oxidative dehydrogenation of ethane (ODE) is limited by the facile deep oxidation and potential safety hazards. Now, electrochemical ODE reaction is incorporated into the anode of a solid oxide electrolysis cell, utilizing the oxygen species generated at anode to catalytically convert ethane. By infiltrating gamma-Al2O3 onto the surface of La0.6Sr0.4Co0.2Fe0.8O3-delta-Sm0.2Ce0.8O2-delta (LSCF-SDC) anode, the ethylene selectivity reaches as high as 92.5 %, while the highest ethane conversion is up to 29.1 % at 600 degrees C with optimized current and ethane flow rate. Density functional theory calculations and in situ X-ray photoelectron spectroscopy characterizations reveal that the Al2O3/LSCF interfaces effectively reduce the amount of adsorbed oxygen species, leading to improved ethylene selectivity and stability, and that the formation of Al-O-Fe alters the electronic structure of interfacial Fe center with increased density of state around Fermi level and downshift of the empty band, which enhances ethane adsorption and conversion.
引用
收藏
页码:16043 / 16046
页数:4
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