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Selective conversion of methane to cyclohexane and hydrogen via efficient hydrogen transfer catalyzed by GaN supported platinum clusters

Non-oxidative liquefaction of methane at room temperature and ambient pressure has long been a scientific “holy grail” of chemical research. Herein, we exploit an unprecedented catalytic transformation of methane exclusively to cyclohexane and hydrogen evolution through effective surface-hydrogen-tr...

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Autores principales: Tan, Lida, Su, Hui, Han, Jingtan, Liu, Mingxin, Li, Chao-Jun
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2022
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9626580/
https://www.ncbi.nlm.nih.gov/pubmed/36319805
http://dx.doi.org/10.1038/s41598-022-21915-9
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author Tan, Lida
Su, Hui
Han, Jingtan
Liu, Mingxin
Li, Chao-Jun
author_facet Tan, Lida
Su, Hui
Han, Jingtan
Liu, Mingxin
Li, Chao-Jun
author_sort Tan, Lida
collection PubMed
description Non-oxidative liquefaction of methane at room temperature and ambient pressure has long been a scientific “holy grail” of chemical research. Herein, we exploit an unprecedented catalytic transformation of methane exclusively to cyclohexane and hydrogen evolution through effective surface-hydrogen-transfer (SHT) at the heterojunctions boundary consisting of electron-rich platinum cluster (Pt) loaded on methane-activating gallium nitride (GaN) host. The experimental analysis demonstrates that the interface-induced overall reaction starts with methane aromatization to benzene and surface-bound hydrogen initiated by the Ga–N pairs, followed by the hydrogenation of benzene to cyclohexane with surface-bound hydrogen. The in-situ activated hydrogen at electron-rich metal Pt cluster is crucial for the hydrogenation and enables an outstanding selectivity (up to 92%) and productivity (41 μmol g(−1)) towards cyclohexane and hydrogen evolution concurrently at 300 °C, which is well-delivered after 5 recycling runs.
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spelling pubmed-96265802022-11-03 Selective conversion of methane to cyclohexane and hydrogen via efficient hydrogen transfer catalyzed by GaN supported platinum clusters Tan, Lida Su, Hui Han, Jingtan Liu, Mingxin Li, Chao-Jun Sci Rep Article Non-oxidative liquefaction of methane at room temperature and ambient pressure has long been a scientific “holy grail” of chemical research. Herein, we exploit an unprecedented catalytic transformation of methane exclusively to cyclohexane and hydrogen evolution through effective surface-hydrogen-transfer (SHT) at the heterojunctions boundary consisting of electron-rich platinum cluster (Pt) loaded on methane-activating gallium nitride (GaN) host. The experimental analysis demonstrates that the interface-induced overall reaction starts with methane aromatization to benzene and surface-bound hydrogen initiated by the Ga–N pairs, followed by the hydrogenation of benzene to cyclohexane with surface-bound hydrogen. The in-situ activated hydrogen at electron-rich metal Pt cluster is crucial for the hydrogenation and enables an outstanding selectivity (up to 92%) and productivity (41 μmol g(−1)) towards cyclohexane and hydrogen evolution concurrently at 300 °C, which is well-delivered after 5 recycling runs. Nature Publishing Group UK 2022-11-01 /pmc/articles/PMC9626580/ /pubmed/36319805 http://dx.doi.org/10.1038/s41598-022-21915-9 Text en © The Author(s) 2022 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 licence, and indicate if changes were made. The images or other third party material in this article are included in the article's Creative Commons licence, unless indicated otherwise in a credit line to the material. If material is not included in the article's Creative Commons licence 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 licence, visit http://creativecommons.org/licenses/by/4.0/ (https://creativecommons.org/licenses/by/4.0/) .
spellingShingle Article
Tan, Lida
Su, Hui
Han, Jingtan
Liu, Mingxin
Li, Chao-Jun
Selective conversion of methane to cyclohexane and hydrogen via efficient hydrogen transfer catalyzed by GaN supported platinum clusters
title Selective conversion of methane to cyclohexane and hydrogen via efficient hydrogen transfer catalyzed by GaN supported platinum clusters
title_full Selective conversion of methane to cyclohexane and hydrogen via efficient hydrogen transfer catalyzed by GaN supported platinum clusters
title_fullStr Selective conversion of methane to cyclohexane and hydrogen via efficient hydrogen transfer catalyzed by GaN supported platinum clusters
title_full_unstemmed Selective conversion of methane to cyclohexane and hydrogen via efficient hydrogen transfer catalyzed by GaN supported platinum clusters
title_short Selective conversion of methane to cyclohexane and hydrogen via efficient hydrogen transfer catalyzed by GaN supported platinum clusters
title_sort selective conversion of methane to cyclohexane and hydrogen via efficient hydrogen transfer catalyzed by gan supported platinum clusters
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9626580/
https://www.ncbi.nlm.nih.gov/pubmed/36319805
http://dx.doi.org/10.1038/s41598-022-21915-9
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