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Selective electrochemical oxidative coupling of methane mediated by Sr(2)Fe(1.5)Mo(0.5)O(6-δ) and its chemical stability

Efficient conversion of methane to value-added products such as olefins and aromatics has been in pursuit for the past few decades. The demand has increased further due to the recent discoveries of shale gas reserves. Oxidative and non-oxidative coupling of methane (OCM and NOCM) have been actively...

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Autores principales: Ramaiyan, Kannan P., Denoyer, Luke H., Benavidez, Angelica, Garzon, Fernando H.
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2021
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9814554/
https://www.ncbi.nlm.nih.gov/pubmed/36697640
http://dx.doi.org/10.1038/s42004-021-00568-1
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author Ramaiyan, Kannan P.
Denoyer, Luke H.
Benavidez, Angelica
Garzon, Fernando H.
author_facet Ramaiyan, Kannan P.
Denoyer, Luke H.
Benavidez, Angelica
Garzon, Fernando H.
author_sort Ramaiyan, Kannan P.
collection PubMed
description Efficient conversion of methane to value-added products such as olefins and aromatics has been in pursuit for the past few decades. The demand has increased further due to the recent discoveries of shale gas reserves. Oxidative and non-oxidative coupling of methane (OCM and NOCM) have been actively researched, although catalysts with commercially viable conversion rates are not yet available. Recently, [Formula: see text] (SFMO-075Fe) has been reported to activate methane in an electrochemical OCM (EC-OCM) set up with a C2 selectivity of 82.2%(1). However, alkaline earth metal-based materials are known to suffer chemical instability in carbon-rich environments. Hence, here we evaluated the chemical stability of SFMO in carbon-rich conditions with varying oxygen concentrations at temperatures relevant for EC-OCM. SFMO-075Fe showed good methane activation properties especially at low overpotentials but suffered poor chemical stability as observed via thermogravimetric, powder XRD, and XPS measurements where SrCO(3) was observed to be a major decomposition product along with SrMoO(3) and MoC. Nevertheless, our study demonstrates that electrochemical methods could be used to selectively activate methane towards partial oxidation products such as ethylene at low overpotentials while higher applied biases result in the complete oxidation of methane to carbon dioxide and water.
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spelling pubmed-98145542023-01-10 Selective electrochemical oxidative coupling of methane mediated by Sr(2)Fe(1.5)Mo(0.5)O(6-δ) and its chemical stability Ramaiyan, Kannan P. Denoyer, Luke H. Benavidez, Angelica Garzon, Fernando H. Commun Chem Article Efficient conversion of methane to value-added products such as olefins and aromatics has been in pursuit for the past few decades. The demand has increased further due to the recent discoveries of shale gas reserves. Oxidative and non-oxidative coupling of methane (OCM and NOCM) have been actively researched, although catalysts with commercially viable conversion rates are not yet available. Recently, [Formula: see text] (SFMO-075Fe) has been reported to activate methane in an electrochemical OCM (EC-OCM) set up with a C2 selectivity of 82.2%(1). However, alkaline earth metal-based materials are known to suffer chemical instability in carbon-rich environments. Hence, here we evaluated the chemical stability of SFMO in carbon-rich conditions with varying oxygen concentrations at temperatures relevant for EC-OCM. SFMO-075Fe showed good methane activation properties especially at low overpotentials but suffered poor chemical stability as observed via thermogravimetric, powder XRD, and XPS measurements where SrCO(3) was observed to be a major decomposition product along with SrMoO(3) and MoC. Nevertheless, our study demonstrates that electrochemical methods could be used to selectively activate methane towards partial oxidation products such as ethylene at low overpotentials while higher applied biases result in the complete oxidation of methane to carbon dioxide and water. Nature Publishing Group UK 2021-09-29 /pmc/articles/PMC9814554/ /pubmed/36697640 http://dx.doi.org/10.1038/s42004-021-00568-1 Text en © The Author(s) 2021 https://creativecommons.org/licenses/by/4.0/Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/ (https://creativecommons.org/licenses/by/4.0/) .
spellingShingle Article
Ramaiyan, Kannan P.
Denoyer, Luke H.
Benavidez, Angelica
Garzon, Fernando H.
Selective electrochemical oxidative coupling of methane mediated by Sr(2)Fe(1.5)Mo(0.5)O(6-δ) and its chemical stability
title Selective electrochemical oxidative coupling of methane mediated by Sr(2)Fe(1.5)Mo(0.5)O(6-δ) and its chemical stability
title_full Selective electrochemical oxidative coupling of methane mediated by Sr(2)Fe(1.5)Mo(0.5)O(6-δ) and its chemical stability
title_fullStr Selective electrochemical oxidative coupling of methane mediated by Sr(2)Fe(1.5)Mo(0.5)O(6-δ) and its chemical stability
title_full_unstemmed Selective electrochemical oxidative coupling of methane mediated by Sr(2)Fe(1.5)Mo(0.5)O(6-δ) and its chemical stability
title_short Selective electrochemical oxidative coupling of methane mediated by Sr(2)Fe(1.5)Mo(0.5)O(6-δ) and its chemical stability
title_sort selective electrochemical oxidative coupling of methane mediated by sr(2)fe(1.5)mo(0.5)o(6-δ) and its chemical stability
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9814554/
https://www.ncbi.nlm.nih.gov/pubmed/36697640
http://dx.doi.org/10.1038/s42004-021-00568-1
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