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


ABSTRACT: 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 (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.

SUBMITTER: Gao Y 

PROVIDER: S-EPMC7182410 | biostudies-literature | 2020 Apr

REPOSITORIES: biostudies-literature

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

Gao Yunfei Y   Wang Xijun X   Liu Junchen J   Huang Chuande C   Zhao Kun K   Zhao Zengli Z   Wang Xiaodong X   Li Fanxing F  

Science advances 20200424 17


Acceptor-doped, redox-active perovskite oxides such as La<sub>0.8</sub>Sr<sub>0.2</sub>FeO<sub>3</sub> (LSF) are active for ethane oxidation to CO <i><sub>x</sub></i> but show poor selectivity to ethylene. This article reports molten Li<sub>2</sub>CO<sub>3</sub> 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 Li<sub>2</sub>CO<sub>3</sub> layer covering the solid LSF sub  ...[more]

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