文献类型：期刊文献

英文题名：Alkali metal halide-coated perovskite redox catalysts for anaerobic oxidative dehydrogenation of n-butane

作者：Gao, Yunfei[1,2];Wang, Xijun[1,3];Corolla, Noel[1];Eldred, Tim[1];Bose, Arnab[1];Gao, Wenpei[1];Li, Fanxing[1]

机构：[1]North Carolina State Univ, Campus Box 7905, Raleigh, NC 27695 USA;[2]East China Univ Sci & Technol, Inst Clean Coal Technol, Shanghai 200237, Peoples R China;[3]Northwestern Univ, Dept Chem & Biol Engn, Evanston, IL 60208 USA

年份：2022

卷号：8

期号：30

外文期刊名：SCIENCE ADVANCES

收录：;EI(收录号：20223112526027);WOS:【SCI-EXPANDED(收录号:WOS:000836554300033)】；

基金：This work was supported by the U.S. NSF (award no. CBET-2116724), the DOE-RAPID Institute (DE-EE007888-05-6), and the Kenan Institute for Engineering, Technology and Science at the NC State University.

语种：英文

外文关键词：Bromine compounds - Catalysts - Chemical bonds - Dehydrogenation - Iron compounds - Lanthanum compounds - Lithium compounds - Metal halides - Molecular dynamics - Reaction intermediates - Reaction kinetics - Redox reactions - Strontium compounds

摘要：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 O-2. This article reports molten LiBr as an effective promoter to modify a redox-active perovskite oxide, i.e., La0.8Sr0.2FeO3 (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.