Alkali metal halide–coated perovskite redox catalysts for anaerobic oxidative dehydrogenation of n-butane

Gao, Yunfei; Wang, Xijun; Corolla, Noel; Eldred, Tim; Bose, Arnab; Gao, Wenpei; Li, Fanxing

doi:10.1126/sciadv.abo7343

Alkali metal halide–coated perovskite redox catalysts for anaerobic oxidative dehydrogenation of n-butane

Journal Article · Wed Jul 27 00:00:00 EDT 2022 · Science Advances

DOI:https://doi.org/10.1126/sciadv.abo7343· OSTI ID:1904809

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North Carolina State University, Raleigh, NC (United States); East China Univ. of Science and Technology, Shanghai (China); North Carolina State Univ., Raleigh, NC (United States)
North Carolina State University, Raleigh, NC (United States); Northwestern Univ., Evanston, IL (United States)
North Carolina State University, Raleigh, NC (United States)

Oxidative dehydrogenation (ODH) of n-butane has the potential to efficiently produce butadiene without equilibrium limitation or coke formation. Despite extensive research efforts, single-pass butadiene yields are limited to <23% in conventional catalytic ODH with gaseous O₂. This article reports molten LiBr as an effective promoter to modify a redox-active perovskite oxide, i.e., La_0.8Sr_0.2FeO₃ (LSF), for chemical looping–oxidative dehydrogenation of n-butane (CL-ODHB). Under the working state, the redox catalyst is composed of a molten LiBr layer covering the solid LSF substrate. Characterizations and ab initio molecular dynamics (AIMD) simulations indicate that peroxide species formed on LSF react with molten LiBr to form active atomic Br, which act as reaction intermediates for C–H bond activation. Meanwhile, molten LiBr layer inhibits unselective CO₂ formation, leading to 42.5% butadiene yield. The redox catalyst design strategy can be extended to CL-ODH of other light alkanes such as iso-butane conversion to iso-butylene, providing a generalized approach for olefin production.

View Accepted Manuscript (DOE)

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

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE); National Science Foundation (NSF)

Grant/Contract Number:: EE0007888

OSTI ID:: 1904809

Journal Information:: Science Advances, Journal Name: Science Advances Journal Issue: 30 Vol. 8; ISSN 2375-2548

Publisher:: AAASCopyright Statement

Country of Publication:: United States

Language:: English

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