Selective conversion of methane to cyclohexane and hydrogen via efficient hydrogen transfer catalyzed by GaN supported platinum clusters
Abstract 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-hy...
| Main Authors: | , , , , |
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| Format: | Article |
| Language: | English |
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Nature Portfolio
2022-11-01
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| Series: | Scientific Reports |
| Online Access: | https://doi.org/10.1038/s41598-022-21915-9 |
| _version_ | 1811223624066007040 |
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| author | Lida Tan Hui Su Jingtan Han Mingxin Liu Chao-Jun Li |
| author_facet | Lida Tan Hui Su Jingtan Han Mingxin Liu Chao-Jun Li |
| author_sort | Lida Tan |
| collection | DOAJ |
| description | Abstract 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. |
| first_indexed | 2024-04-12T08:35:58Z |
| format | Article |
| id | doaj.art-15e85cd6eb654b1483559de0a9ad271b |
| institution | Directory Open Access Journal |
| issn | 2045-2322 |
| language | English |
| last_indexed | 2024-04-12T08:35:58Z |
| publishDate | 2022-11-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Scientific Reports |
| spelling | doaj.art-15e85cd6eb654b1483559de0a9ad271b2022-12-22T03:40:00ZengNature PortfolioScientific Reports2045-23222022-11-011211810.1038/s41598-022-21915-9Selective conversion of methane to cyclohexane and hydrogen via efficient hydrogen transfer catalyzed by GaN supported platinum clustersLida Tan0Hui Su1Jingtan Han2Mingxin Liu3Chao-Jun Li4Department of Chemistry, and FQRNT Centre for Green Chemistry and Catalysis, McGill UniversityDepartment of Chemistry, and FQRNT Centre for Green Chemistry and Catalysis, McGill UniversityDepartment of Chemistry, and FQRNT Centre for Green Chemistry and Catalysis, McGill UniversityDepartment of Chemistry, and FQRNT Centre for Green Chemistry and Catalysis, McGill UniversityDepartment of Chemistry, and FQRNT Centre for Green Chemistry and Catalysis, McGill UniversityAbstract 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.https://doi.org/10.1038/s41598-022-21915-9 |
| spellingShingle | Lida Tan Hui Su Jingtan Han Mingxin Liu Chao-Jun Li Selective conversion of methane to cyclohexane and hydrogen via efficient hydrogen transfer catalyzed by GaN supported platinum clusters Scientific Reports |
| 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 |
| url | https://doi.org/10.1038/s41598-022-21915-9 |
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