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High-efficiency direct methane conversion to oxygenates on a cerium dioxide nanowires supported rhodium single-atom catalyst

Direct methane conversion (DMC) to high value-added products is of significant importance for the effective utilization of CH(4) to combat the energy crisis. However, there are ongoing challenges in DMC associated with the selective C−H activation of CH(4). The quest for high-efficiency catalysts fo...

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Autores principales: Bai, Shuxing, Liu, Fangfang, Huang, Bolong, Li, Fan, Lin, Haiping, Wu, Tong, Sun, Mingzi, Wu, Jianbo, Shao, Qi, Xu, Yong, Huang, Xiaoqing
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2020
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC7031227/
https://www.ncbi.nlm.nih.gov/pubmed/32075982
http://dx.doi.org/10.1038/s41467-020-14742-x
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author Bai, Shuxing
Liu, Fangfang
Huang, Bolong
Li, Fan
Lin, Haiping
Wu, Tong
Sun, Mingzi
Wu, Jianbo
Shao, Qi
Xu, Yong
Huang, Xiaoqing
author_facet Bai, Shuxing
Liu, Fangfang
Huang, Bolong
Li, Fan
Lin, Haiping
Wu, Tong
Sun, Mingzi
Wu, Jianbo
Shao, Qi
Xu, Yong
Huang, Xiaoqing
author_sort Bai, Shuxing
collection PubMed
description Direct methane conversion (DMC) to high value-added products is of significant importance for the effective utilization of CH(4) to combat the energy crisis. However, there are ongoing challenges in DMC associated with the selective C−H activation of CH(4). The quest for high-efficiency catalysts for this process is limited by the current drawbacks including poor activity and low selectivity. Here we show a cerium dioxide (CeO(2)) nanowires supported rhodium (Rh) single-atom (SAs Rh-CeO(2) NWs) that can serve as a high-efficiency catalyst for DMC to oxygenates (i.e., CH(3)OH and CH(3)OOH) under mild conditions. Compared to Rh/CeO(2) nanowires (Rh clusters) prepared by a conventional wet-impregnation method, CeO(2) nanowires supported Rh single-atom exhibits 6.5 times higher of the oxygenates yield (1231.7 vs. 189.4 mmol g(Rh)(−1) h(−1)), which largely outperforms that of the reported catalysts in the same class. This work demonstrates a highly efficient DMC process and promotes the research on Rh single-atom catalysts in heterogeneous catalysis.
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spelling pubmed-70312272020-03-04 High-efficiency direct methane conversion to oxygenates on a cerium dioxide nanowires supported rhodium single-atom catalyst Bai, Shuxing Liu, Fangfang Huang, Bolong Li, Fan Lin, Haiping Wu, Tong Sun, Mingzi Wu, Jianbo Shao, Qi Xu, Yong Huang, Xiaoqing Nat Commun Article Direct methane conversion (DMC) to high value-added products is of significant importance for the effective utilization of CH(4) to combat the energy crisis. However, there are ongoing challenges in DMC associated with the selective C−H activation of CH(4). The quest for high-efficiency catalysts for this process is limited by the current drawbacks including poor activity and low selectivity. Here we show a cerium dioxide (CeO(2)) nanowires supported rhodium (Rh) single-atom (SAs Rh-CeO(2) NWs) that can serve as a high-efficiency catalyst for DMC to oxygenates (i.e., CH(3)OH and CH(3)OOH) under mild conditions. Compared to Rh/CeO(2) nanowires (Rh clusters) prepared by a conventional wet-impregnation method, CeO(2) nanowires supported Rh single-atom exhibits 6.5 times higher of the oxygenates yield (1231.7 vs. 189.4 mmol g(Rh)(−1) h(−1)), which largely outperforms that of the reported catalysts in the same class. This work demonstrates a highly efficient DMC process and promotes the research on Rh single-atom catalysts in heterogeneous catalysis. Nature Publishing Group UK 2020-02-19 /pmc/articles/PMC7031227/ /pubmed/32075982 http://dx.doi.org/10.1038/s41467-020-14742-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
Bai, Shuxing
Liu, Fangfang
Huang, Bolong
Li, Fan
Lin, Haiping
Wu, Tong
Sun, Mingzi
Wu, Jianbo
Shao, Qi
Xu, Yong
Huang, Xiaoqing
High-efficiency direct methane conversion to oxygenates on a cerium dioxide nanowires supported rhodium single-atom catalyst
title High-efficiency direct methane conversion to oxygenates on a cerium dioxide nanowires supported rhodium single-atom catalyst
title_full High-efficiency direct methane conversion to oxygenates on a cerium dioxide nanowires supported rhodium single-atom catalyst
title_fullStr High-efficiency direct methane conversion to oxygenates on a cerium dioxide nanowires supported rhodium single-atom catalyst
title_full_unstemmed High-efficiency direct methane conversion to oxygenates on a cerium dioxide nanowires supported rhodium single-atom catalyst
title_short High-efficiency direct methane conversion to oxygenates on a cerium dioxide nanowires supported rhodium single-atom catalyst
title_sort high-efficiency direct methane conversion to oxygenates on a cerium dioxide nanowires supported rhodium single-atom catalyst
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC7031227/
https://www.ncbi.nlm.nih.gov/pubmed/32075982
http://dx.doi.org/10.1038/s41467-020-14742-x
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