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PdCu nanoalloy decorated photocatalysts for efficient and selective oxidative coupling of methane in flow reactors

Methane activation by photocatalysis is one of the promising sustainable technologies for chemical synthesis. However, the current efficiency and stability of the process are moderate. Herein, a PdCu nanoalloy (~2.3 nm) was decorated on TiO(2), which works for the efficient, stable, and selective ph...

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Autores principales: Li, Xiyi, Wang, Chao, Yang, Jianlong, Xu, Youxun, Yang, Yi, Yu, Jiaguo, Delgado, Juan J., Martsinovich, Natalia, Sun, Xiao, Zheng, Xu-Sheng, Huang, Weixin, Tang, Junwang
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2023
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10564738/
https://www.ncbi.nlm.nih.gov/pubmed/37816721
http://dx.doi.org/10.1038/s41467-023-41996-y
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author Li, Xiyi
Wang, Chao
Yang, Jianlong
Xu, Youxun
Yang, Yi
Yu, Jiaguo
Delgado, Juan J.
Martsinovich, Natalia
Sun, Xiao
Zheng, Xu-Sheng
Huang, Weixin
Tang, Junwang
author_facet Li, Xiyi
Wang, Chao
Yang, Jianlong
Xu, Youxun
Yang, Yi
Yu, Jiaguo
Delgado, Juan J.
Martsinovich, Natalia
Sun, Xiao
Zheng, Xu-Sheng
Huang, Weixin
Tang, Junwang
author_sort Li, Xiyi
collection PubMed
description Methane activation by photocatalysis is one of the promising sustainable technologies for chemical synthesis. However, the current efficiency and stability of the process are moderate. Herein, a PdCu nanoalloy (~2.3 nm) was decorated on TiO(2), which works for the efficient, stable, and selective photocatalytic oxidative coupling of methane at room temperature. A high methane conversion rate of 2480 μmol g(−1) h(−1) to C(2) with an apparent quantum efficiency of ~8.4% has been achieved. More importantly, the photocatalyst exhibits the turnover frequency and turnover number of 116 h(−1) and 12,642 with respect to PdCu, representing a record among all the photocatalytic processes (λ > 300 nm) operated at room temperature, together with a long stability of over 112 hours. The nanoalloy works as a hole acceptor, in which Pd softens and weakens C-H bond in methane and Cu decreases the adsorption energy of C(2) products, leading to the high efficiency and long-time stability.
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spelling pubmed-105647382023-10-12 PdCu nanoalloy decorated photocatalysts for efficient and selective oxidative coupling of methane in flow reactors Li, Xiyi Wang, Chao Yang, Jianlong Xu, Youxun Yang, Yi Yu, Jiaguo Delgado, Juan J. Martsinovich, Natalia Sun, Xiao Zheng, Xu-Sheng Huang, Weixin Tang, Junwang Nat Commun Article Methane activation by photocatalysis is one of the promising sustainable technologies for chemical synthesis. However, the current efficiency and stability of the process are moderate. Herein, a PdCu nanoalloy (~2.3 nm) was decorated on TiO(2), which works for the efficient, stable, and selective photocatalytic oxidative coupling of methane at room temperature. A high methane conversion rate of 2480 μmol g(−1) h(−1) to C(2) with an apparent quantum efficiency of ~8.4% has been achieved. More importantly, the photocatalyst exhibits the turnover frequency and turnover number of 116 h(−1) and 12,642 with respect to PdCu, representing a record among all the photocatalytic processes (λ > 300 nm) operated at room temperature, together with a long stability of over 112 hours. The nanoalloy works as a hole acceptor, in which Pd softens and weakens C-H bond in methane and Cu decreases the adsorption energy of C(2) products, leading to the high efficiency and long-time stability. Nature Publishing Group UK 2023-10-10 /pmc/articles/PMC10564738/ /pubmed/37816721 http://dx.doi.org/10.1038/s41467-023-41996-y Text en © The Author(s) 2023 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
Li, Xiyi
Wang, Chao
Yang, Jianlong
Xu, Youxun
Yang, Yi
Yu, Jiaguo
Delgado, Juan J.
Martsinovich, Natalia
Sun, Xiao
Zheng, Xu-Sheng
Huang, Weixin
Tang, Junwang
PdCu nanoalloy decorated photocatalysts for efficient and selective oxidative coupling of methane in flow reactors
title PdCu nanoalloy decorated photocatalysts for efficient and selective oxidative coupling of methane in flow reactors
title_full PdCu nanoalloy decorated photocatalysts for efficient and selective oxidative coupling of methane in flow reactors
title_fullStr PdCu nanoalloy decorated photocatalysts for efficient and selective oxidative coupling of methane in flow reactors
title_full_unstemmed PdCu nanoalloy decorated photocatalysts for efficient and selective oxidative coupling of methane in flow reactors
title_short PdCu nanoalloy decorated photocatalysts for efficient and selective oxidative coupling of methane in flow reactors
title_sort pdcu nanoalloy decorated photocatalysts for efficient and selective oxidative coupling of methane in flow reactors
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10564738/
https://www.ncbi.nlm.nih.gov/pubmed/37816721
http://dx.doi.org/10.1038/s41467-023-41996-y
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