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A molten carbonate shell modified perovskite redox catalyst for anaerobic oxidative dehydrogenation of ethane
Acceptor-doped, redox-active perovskite oxides such as La(0.8)Sr(0.2)FeO(3) (LSF) are active for ethane oxidation to CO(x) but show poor selectivity to ethylene. This article reports molten Li(2)CO(3) as an effective “promoter” to modify LSF for chemical looping–oxidative dehydrogenation (CL-ODH) of...
Autores principales: | , , , , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
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American Association for the Advancement of Science
2020
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Materias: | |
Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC7182410/ https://www.ncbi.nlm.nih.gov/pubmed/32426468 http://dx.doi.org/10.1126/sciadv.aaz9339 |
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author | Gao, Yunfei Wang, Xijun Liu, Junchen Huang, Chuande Zhao, Kun Zhao, Zengli Wang, Xiaodong Li, Fanxing |
author_facet | Gao, Yunfei Wang, Xijun Liu, Junchen Huang, Chuande Zhao, Kun Zhao, Zengli Wang, Xiaodong Li, Fanxing |
author_sort | Gao, Yunfei |
collection | PubMed |
description | Acceptor-doped, redox-active perovskite oxides such as La(0.8)Sr(0.2)FeO(3) (LSF) are active for ethane oxidation to CO(x) but show poor selectivity to ethylene. This article reports molten Li(2)CO(3) 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(2)CO(3) 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 Fe(4+)→Fe(3+) 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. |
format | Online Article Text |
id | pubmed-7182410 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2020 |
publisher | American Association for the Advancement of Science |
record_format | MEDLINE/PubMed |
spelling | pubmed-71824102020-05-18 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 Sci Adv Research Articles Acceptor-doped, redox-active perovskite oxides such as La(0.8)Sr(0.2)FeO(3) (LSF) are active for ethane oxidation to CO(x) but show poor selectivity to ethylene. This article reports molten Li(2)CO(3) 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(2)CO(3) 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 Fe(4+)→Fe(3+) 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. American Association for the Advancement of Science 2020-04-24 /pmc/articles/PMC7182410/ /pubmed/32426468 http://dx.doi.org/10.1126/sciadv.aaz9339 Text en Copyright © 2020 The Authors, some rights reserved; exclusive licensee American Association for the Advancement of Science. No claim to original U.S. Government Works. Distributed under a Creative Commons Attribution NonCommercial License 4.0 (CC BY-NC). http://creativecommons.org/licenses/by-nc/4.0/ This is an open-access article distributed under the terms of the Creative Commons Attribution-NonCommercial license (http://creativecommons.org/licenses/by-nc/4.0/) , which permits use, distribution, and reproduction in any medium, so long as the resultant use is not for commercial advantage and provided the original work is properly cited. |
spellingShingle | Research Articles Gao, Yunfei Wang, Xijun Liu, Junchen Huang, Chuande Zhao, Kun Zhao, Zengli Wang, Xiaodong Li, Fanxing A molten carbonate shell modified perovskite redox catalyst for anaerobic oxidative dehydrogenation of ethane |
title | A molten carbonate shell modified perovskite redox catalyst for anaerobic oxidative dehydrogenation of ethane |
title_full | A molten carbonate shell modified perovskite redox catalyst for anaerobic oxidative dehydrogenation of ethane |
title_fullStr | A molten carbonate shell modified perovskite redox catalyst for anaerobic oxidative dehydrogenation of ethane |
title_full_unstemmed | A molten carbonate shell modified perovskite redox catalyst for anaerobic oxidative dehydrogenation of ethane |
title_short | A molten carbonate shell modified perovskite redox catalyst for anaerobic oxidative dehydrogenation of ethane |
title_sort | molten carbonate shell modified perovskite redox catalyst for anaerobic oxidative dehydrogenation of ethane |
topic | Research Articles |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC7182410/ https://www.ncbi.nlm.nih.gov/pubmed/32426468 http://dx.doi.org/10.1126/sciadv.aaz9339 |
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