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A molten carbonate shell modified perovskite redox catalyst for anaerobic oxidative dehydrogenation of ethane
Gao, Yunfei1; Wang, Xijun1; Liu, Junchen1; Huang, Chuande2; Zhao, Kun3; Zhao, Zengli3; Wang, Xiaodong2; Li, Fanxing1
2020-04-01
发表期刊SCIENCE ADVANCES
ISSN2375-2548
卷号6期号:17页码:10
通讯作者Li, Fanxing(fli5@ncsu.edu)
摘要Acceptor-doped, redox-active perovskite oxides such as La0.8Sr0.2FeO3 (LSF) are active for ethane oxidation to CO X but show poor selectivity to ethylene. This article reports molten Li2CO3 as an effective "promoter" to modify LSF for chemical looping-oxidative dehydrogenation (CL-ODH) of ethane. Under the working state, the redox catalyst is composed of a molten Li2CO3 layer covering the solid LSF substrate. The molten layer facilitates the transport of active peroxide (O-2(2-)) species formed on LSF while blocking the nonselective sites. Spectroscopy measurements and density functional theory calculations indicate that Fe4+ -> Fe3+ transition is responsible for the peroxide formation, which results in both exothermic ODH and air reoxidation steps. With >90% ethylene selectivity, up to 59% ethylene yield, and favorable heat of reactions, the core-shell redox catalyst has an excellent potential to be effective for intensified ethane conversion. The mechanistic findings also provide a generalized approach for designing CL-ODH redox catalysts.
DOI10.1126/sciadv.aaz9339
关键词[WOS]INTENSIFIED ETHYLENE PRODUCTION ; LATTICE OXYGEN ; METAL-OXIDES ; PROMOTERS ; SURFACE ; SYSTEM ; PHASE
收录类别SCI
语种英语
资助项目U.S. NSF[CBET-1604605] ; DOE-RAPID Institute[DE-EE007888-05-6] ; Kenan Institute for Engineering, Technology and Science at the NC State University
WOS研究方向Science & Technology - Other Topics
项目资助者U.S. NSF ; DOE-RAPID Institute ; Kenan Institute for Engineering, Technology and Science at the NC State University
WOS类目Multidisciplinary Sciences
WOS记录号WOS:000530628100041
出版者AMER ASSOC ADVANCEMENT SCIENCE
引用统计
被引频次:56[WOS]   [WOS记录]     [WOS相关记录]
文献类型期刊论文
条目标识符http://ir.giec.ac.cn/handle/344007/26951
专题中国科学院广州能源研究所
通讯作者Li, Fanxing
作者单位1.North Carolina State Univ, Campus Box 7905, Raleigh, NC 27695 USA
2.Chinese Acad Sci, Dalian Inst Chem Phys, Dalian, Peoples R China
3.Chinese Acad Sci, Guangzhou Inst Energy Convers, Guangzhou, Peoples R China
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Gao, Yunfei,Wang, Xijun,Liu, Junchen,et al. A molten carbonate shell modified perovskite redox catalyst for anaerobic oxidative dehydrogenation of ethane[J]. SCIENCE ADVANCES,2020,6(17):10.
APA Gao, Yunfei.,Wang, Xijun.,Liu, Junchen.,Huang, Chuande.,Zhao, Kun.,...&Li, Fanxing.(2020).A molten carbonate shell modified perovskite redox catalyst for anaerobic oxidative dehydrogenation of ethane.SCIENCE ADVANCES,6(17),10.
MLA Gao, Yunfei,et al."A molten carbonate shell modified perovskite redox catalyst for anaerobic oxidative dehydrogenation of ethane".SCIENCE ADVANCES 6.17(2020):10.
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