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Reactions of CO(2) and ethane enable CO bond insertion for production of C3 oxygenates

Reacting CO(2) and ethane to synthesize value-added oxygenate molecules represents opportunities to simultaneously reduce CO(2) emissions and upgrade underutilized ethane in shale gas. Herein, we propose a strategy to produce C3 oxygenates using a tandem reactor. This strategy is achieved with a Fe(...

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Autores principales: Xie, Zhenhua, Xu, Yuanguo, Xie, Meng, Chen, Xiaobo, Lee, Ji Hoon, Stavitski, Eli, Kattel, Shyam, Chen, Jingguang G.
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2020
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC7170877/
https://www.ncbi.nlm.nih.gov/pubmed/32313008
http://dx.doi.org/10.1038/s41467-020-15849-x
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author Xie, Zhenhua
Xu, Yuanguo
Xie, Meng
Chen, Xiaobo
Lee, Ji Hoon
Stavitski, Eli
Kattel, Shyam
Chen, Jingguang G.
author_facet Xie, Zhenhua
Xu, Yuanguo
Xie, Meng
Chen, Xiaobo
Lee, Ji Hoon
Stavitski, Eli
Kattel, Shyam
Chen, Jingguang G.
author_sort Xie, Zhenhua
collection PubMed
description Reacting CO(2) and ethane to synthesize value-added oxygenate molecules represents opportunities to simultaneously reduce CO(2) emissions and upgrade underutilized ethane in shale gas. Herein, we propose a strategy to produce C3 oxygenates using a tandem reactor. This strategy is achieved with a Fe(3)Ni(1)/CeO(2) catalyst (first reactor at 600–800 °C) for CO(2)-assisted dehydrogenation and reforming of ethane to produce ethylene, CO, and H(2), and a RhCo(x)/MCM-41 catalyst (second reactor at 200 °C) enabling CO insertion for the production of C3 oxygenates (propanal and 1-propanol) via the heterogeneous hydroformylation reaction at ambient pressure. In-situ characterization using synchrotron spectroscopies and density functional theory (DFT) calculations reveal the effect of Rh–Co bimetallic formation in facilitating the production of C3 oxygenates. The proposed strategy provides an opportunity for upgrading light alkanes in shale gas by reacting with CO(2) to produce aldehydes and alcohols.
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spelling pubmed-71708772020-04-23 Reactions of CO(2) and ethane enable CO bond insertion for production of C3 oxygenates Xie, Zhenhua Xu, Yuanguo Xie, Meng Chen, Xiaobo Lee, Ji Hoon Stavitski, Eli Kattel, Shyam Chen, Jingguang G. Nat Commun Article Reacting CO(2) and ethane to synthesize value-added oxygenate molecules represents opportunities to simultaneously reduce CO(2) emissions and upgrade underutilized ethane in shale gas. Herein, we propose a strategy to produce C3 oxygenates using a tandem reactor. This strategy is achieved with a Fe(3)Ni(1)/CeO(2) catalyst (first reactor at 600–800 °C) for CO(2)-assisted dehydrogenation and reforming of ethane to produce ethylene, CO, and H(2), and a RhCo(x)/MCM-41 catalyst (second reactor at 200 °C) enabling CO insertion for the production of C3 oxygenates (propanal and 1-propanol) via the heterogeneous hydroformylation reaction at ambient pressure. In-situ characterization using synchrotron spectroscopies and density functional theory (DFT) calculations reveal the effect of Rh–Co bimetallic formation in facilitating the production of C3 oxygenates. The proposed strategy provides an opportunity for upgrading light alkanes in shale gas by reacting with CO(2) to produce aldehydes and alcohols. Nature Publishing Group UK 2020-04-20 /pmc/articles/PMC7170877/ /pubmed/32313008 http://dx.doi.org/10.1038/s41467-020-15849-x Text en © The Author(s) 2020 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/.
spellingShingle Article
Xie, Zhenhua
Xu, Yuanguo
Xie, Meng
Chen, Xiaobo
Lee, Ji Hoon
Stavitski, Eli
Kattel, Shyam
Chen, Jingguang G.
Reactions of CO(2) and ethane enable CO bond insertion for production of C3 oxygenates
title Reactions of CO(2) and ethane enable CO bond insertion for production of C3 oxygenates
title_full Reactions of CO(2) and ethane enable CO bond insertion for production of C3 oxygenates
title_fullStr Reactions of CO(2) and ethane enable CO bond insertion for production of C3 oxygenates
title_full_unstemmed Reactions of CO(2) and ethane enable CO bond insertion for production of C3 oxygenates
title_short Reactions of CO(2) and ethane enable CO bond insertion for production of C3 oxygenates
title_sort reactions of co(2) and ethane enable co bond insertion for production of c3 oxygenates
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC7170877/
https://www.ncbi.nlm.nih.gov/pubmed/32313008
http://dx.doi.org/10.1038/s41467-020-15849-x
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