PdCu nanoalloy decorated photocatalysts for efficient and selective oxidative coupling of methane in flow reactors
Abstract 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 TiO2, which works for the efficient, stable, and selec...
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| Format: | Article |
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Nature Portfolio
2023-10-01
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| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-023-41996-y |
| _version_ | 1827709939799293952 |
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| author | Xiyi Li Chao Wang Jianlong Yang Youxun Xu Yi Yang Jiaguo Yu Juan J. Delgado Natalia Martsinovich Xiao Sun Xu-Sheng Zheng Weixin Huang Junwang Tang |
| author_facet | Xiyi Li Chao Wang Jianlong Yang Youxun Xu Yi Yang Jiaguo Yu Juan J. Delgado Natalia Martsinovich Xiao Sun Xu-Sheng Zheng Weixin Huang Junwang Tang |
| author_sort | Xiyi Li |
| collection | DOAJ |
| description | Abstract 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 TiO2, 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 C2 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 C2 products, leading to the high efficiency and long-time stability. |
| first_indexed | 2024-03-10T17:30:16Z |
| format | Article |
| id | doaj.art-0501d9447f494bcfbdfc43303c3e74c6 |
| institution | Directory Open Access Journal |
| issn | 2041-1723 |
| language | English |
| last_indexed | 2024-03-10T17:30:16Z |
| publishDate | 2023-10-01 |
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| record_format | Article |
| series | Nature Communications |
| spelling | doaj.art-0501d9447f494bcfbdfc43303c3e74c62023-11-20T10:02:23ZengNature PortfolioNature Communications2041-17232023-10-0114111310.1038/s41467-023-41996-yPdCu nanoalloy decorated photocatalysts for efficient and selective oxidative coupling of methane in flow reactorsXiyi Li0Chao Wang1Jianlong Yang2Youxun Xu3Yi Yang4Jiaguo Yu5Juan J. Delgado6Natalia Martsinovich7Xiao Sun8Xu-Sheng Zheng9Weixin Huang10Junwang Tang11Department of Chemical Engineering, University College LondonDepartment of Chemical Engineering, University College LondonKey Lab of Synthetic and Natural Functional Molecule Chemistry of Ministry of Education, the Energy and Catalysis Hub, College of Chemistry and Materials Science, Northwest UniversityDepartment of Chemical Engineering, University College LondonState Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of TechnologyLaboratory of Solar Fuel, Faculty of Materials Science and Chemistry, China University of GeosciencesDepartamento de Ciencia de los Materiales e Ingeniería Metalúrgica y Química Inorgánica, Facultad de Ciencias, Universidad de Cádiz, Campus Rio San PedroDepartment of Chemistry, University of SheffieldHefei National Research Center for Physical Sciences at the Microscale, iChEM, Key Laboratory of Surface and Interface Chemistry and Energy Catalysis of Anhui Higher Education Institutes, School of Chemistry and Materials Science, University of Science and Technology of ChinaNational Synchrotron Radiation Laboratory, University of Science and Technology of ChinaHefei National Research Center for Physical Sciences at the Microscale, iChEM, Key Laboratory of Surface and Interface Chemistry and Energy Catalysis of Anhui Higher Education Institutes, School of Chemistry and Materials Science, University of Science and Technology of ChinaDepartment of Chemical Engineering, University College LondonAbstract 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 TiO2, 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 C2 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 C2 products, leading to the high efficiency and long-time stability.https://doi.org/10.1038/s41467-023-41996-y |
| spellingShingle | Xiyi Li Chao Wang Jianlong Yang Youxun Xu Yi Yang Jiaguo Yu Juan J. Delgado Natalia Martsinovich Xiao Sun Xu-Sheng Zheng Weixin Huang Junwang Tang PdCu nanoalloy decorated photocatalysts for efficient and selective oxidative coupling of methane in flow reactors Nature Communications |
| 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 |
| url | https://doi.org/10.1038/s41467-023-41996-y |
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