A molten carbonate shell modified perovskite redox catalyst for anaerobic oxidative dehydrogenation of ethane

Gao, Yunfei; Wang, Xijun; Liu, Junchen; Huang, Chuande; Zhao, Kun; Zhao, Zengli; Wang, Xiaodong; Li, Fanxing

doi:10.1126/sciadv.aaz9339

Title: A molten carbonate shell modified perovskite redox catalyst for anaerobic oxidative dehydrogenation of ethane

Journal Article · Fri Apr 24 00:00:00 EDT 2020 · Science Advances

DOI:https://doi.org/10.1126/sciadv.aaz9339· OSTI ID:1803998

^[1];

^[1]; Liu, Junchen ^[1];

^[2]; Zhao, Kun ^[3]; Zhao, Zengli ^[3];

^[2];

^[1]

North Carolina State Univ., Raleigh, NC (United States)
Chinese Academy of Sciences, Dalian (China). Dalian Inst. of Chemical Physics
Chinese Academy of Sciences, Guangzhou (China). Guangzhou Inst. of Energy Conversion

Acceptor-doped, redox-active perovskite oxides such as La_0.8Sr_0.2FeO₃(LSF) are active for ethane oxidation to CO_xbut show poor selectivity to ethylene. This article reports molten Li₂CO₃as 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 Li₂CO₃layer covering the solid LSF substrate. The molten layer facilitates the transport of active peroxide (O₂^2-) 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.

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Research Organization:: American Institute of Chemical Engineers (AIChE), New York, NY (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE)

Grant/Contract Number:: EE0007888

OSTI ID:: 1803998

Journal Information:: Science Advances, Vol. 6, Issue 17; ISSN 2375-2548

Publisher:: AAASCopyright Statement

Country of Publication:: United States

Language:: English

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