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Understanding the Impact of Hydrogen Activation by SrCe(0.8)Zr(0.2)O(3−δ) Perovskite Membrane Material on Direct Non-Oxidative Methane Conversion

Direct non-oxidative methane conversion (DNMC) converts methane (CH(4)) in one step to olefin and aromatic hydrocarbons and hydrogen (H(2)) co-product. Membrane reactors comprising methane activation catalysts and H(2)-permeable membranes can enhance methane conversion by in situ H(2) removal via Le...

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Autores principales: Cheng, Sichao, Oh, Su Cheun, Sakbodin, Mann, Qiu, Limei, Diao, Yuxia, Liu, Dongxia
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Frontiers Media S.A. 2022
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8784877/
https://www.ncbi.nlm.nih.gov/pubmed/35083196
http://dx.doi.org/10.3389/fchem.2021.806464
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author Cheng, Sichao
Oh, Su Cheun
Sakbodin, Mann
Qiu, Limei
Diao, Yuxia
Liu, Dongxia
author_facet Cheng, Sichao
Oh, Su Cheun
Sakbodin, Mann
Qiu, Limei
Diao, Yuxia
Liu, Dongxia
author_sort Cheng, Sichao
collection PubMed
description Direct non-oxidative methane conversion (DNMC) converts methane (CH(4)) in one step to olefin and aromatic hydrocarbons and hydrogen (H(2)) co-product. Membrane reactors comprising methane activation catalysts and H(2)-permeable membranes can enhance methane conversion by in situ H(2) removal via Le Chatelier's principle. Rigorous description of H(2) kinetic effects on both membrane and catalyst materials in the membrane reactor, however, has been rarely studied. In this work, we report the impact of hydrogen activation by hydrogen-permeable SrCe(0.8)Zr(0.2)O(3−δ) (SCZO) perovskite oxide material on DNMC over an iron/silica catalyst. The SCZO oxide has mixed ionic and electronic conductivity and is capable of H(2) activation into protons and electrons for H(2) permeation. In the fixed-bed reactor packed with a mixture of SCZO oxide and iron/silica catalyst, stable and high methane conversion and low coke selectivity in DNMC was achieved by co-feeding of H(2) in methane stream. The characterizations show that SCZO activates H(2) to favor “soft coke” formation on the catalyst. The SCZO could absorb H(2) in situ to lower its local concentration to mitigate the reverse reaction of DNMC in the tested conditions. The co-existence of H(2) co-feed, SCZO oxide, and DNMC catalyst in the present study mimics the conditions of DNMC in the H(2)-permeable SCZO membrane reactor. The findings in this work offer the mechanistic understanding of and guidance for the design of H(2)-permeable membrane reactors for DNMC and other alkane dehydrogenation reactions.
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spelling pubmed-87848772022-01-25 Understanding the Impact of Hydrogen Activation by SrCe(0.8)Zr(0.2)O(3−δ) Perovskite Membrane Material on Direct Non-Oxidative Methane Conversion Cheng, Sichao Oh, Su Cheun Sakbodin, Mann Qiu, Limei Diao, Yuxia Liu, Dongxia Front Chem Chemistry Direct non-oxidative methane conversion (DNMC) converts methane (CH(4)) in one step to olefin and aromatic hydrocarbons and hydrogen (H(2)) co-product. Membrane reactors comprising methane activation catalysts and H(2)-permeable membranes can enhance methane conversion by in situ H(2) removal via Le Chatelier's principle. Rigorous description of H(2) kinetic effects on both membrane and catalyst materials in the membrane reactor, however, has been rarely studied. In this work, we report the impact of hydrogen activation by hydrogen-permeable SrCe(0.8)Zr(0.2)O(3−δ) (SCZO) perovskite oxide material on DNMC over an iron/silica catalyst. The SCZO oxide has mixed ionic and electronic conductivity and is capable of H(2) activation into protons and electrons for H(2) permeation. In the fixed-bed reactor packed with a mixture of SCZO oxide and iron/silica catalyst, stable and high methane conversion and low coke selectivity in DNMC was achieved by co-feeding of H(2) in methane stream. The characterizations show that SCZO activates H(2) to favor “soft coke” formation on the catalyst. The SCZO could absorb H(2) in situ to lower its local concentration to mitigate the reverse reaction of DNMC in the tested conditions. The co-existence of H(2) co-feed, SCZO oxide, and DNMC catalyst in the present study mimics the conditions of DNMC in the H(2)-permeable SCZO membrane reactor. The findings in this work offer the mechanistic understanding of and guidance for the design of H(2)-permeable membrane reactors for DNMC and other alkane dehydrogenation reactions. Frontiers Media S.A. 2022-01-10 /pmc/articles/PMC8784877/ /pubmed/35083196 http://dx.doi.org/10.3389/fchem.2021.806464 Text en Copyright © 2022 Cheng, Oh, Sakbodin, Qiu, Diao and Liu. https://creativecommons.org/licenses/by/4.0/This is an open-access article distributed under the terms of the Creative Commons Attribution License (CC BY). The use, distribution or reproduction in other forums is permitted, provided the original author(s) and the copyright owner(s) are credited and that the original publication in this journal is cited, in accordance with accepted academic practice. No use, distribution or reproduction is permitted which does not comply with these terms.
spellingShingle Chemistry
Cheng, Sichao
Oh, Su Cheun
Sakbodin, Mann
Qiu, Limei
Diao, Yuxia
Liu, Dongxia
Understanding the Impact of Hydrogen Activation by SrCe(0.8)Zr(0.2)O(3−δ) Perovskite Membrane Material on Direct Non-Oxidative Methane Conversion
title Understanding the Impact of Hydrogen Activation by SrCe(0.8)Zr(0.2)O(3−δ) Perovskite Membrane Material on Direct Non-Oxidative Methane Conversion
title_full Understanding the Impact of Hydrogen Activation by SrCe(0.8)Zr(0.2)O(3−δ) Perovskite Membrane Material on Direct Non-Oxidative Methane Conversion
title_fullStr Understanding the Impact of Hydrogen Activation by SrCe(0.8)Zr(0.2)O(3−δ) Perovskite Membrane Material on Direct Non-Oxidative Methane Conversion
title_full_unstemmed Understanding the Impact of Hydrogen Activation by SrCe(0.8)Zr(0.2)O(3−δ) Perovskite Membrane Material on Direct Non-Oxidative Methane Conversion
title_short Understanding the Impact of Hydrogen Activation by SrCe(0.8)Zr(0.2)O(3−δ) Perovskite Membrane Material on Direct Non-Oxidative Methane Conversion
title_sort understanding the impact of hydrogen activation by srce(0.8)zr(0.2)o(3−δ) perovskite membrane material on direct non-oxidative methane conversion
topic Chemistry
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8784877/
https://www.ncbi.nlm.nih.gov/pubmed/35083196
http://dx.doi.org/10.3389/fchem.2021.806464
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