Silver and Copper Dual Single Atoms Boosting Direct Oxidation of Methane to Methanol via Synergistic Catalysis
Abstract Rationally constructing atom‐precise active sites is highly important to promote their catalytic performance but still challenging. Herein, this work designs and constructs ZSM‐5 supported Cu and Ag dual single atoms as a proof‐of‐concept catalyst (Ag1−Cu1/ZSM‐5 hetero‐SAC (single‐atom cata...
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| Format: | Article |
| Language: | English |
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Wiley
2023-09-01
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| Series: | Advanced Science |
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| Online Access: | https://doi.org/10.1002/advs.202302143 |
| _version_ | 1797684968019722240 |
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| author | Baiyang Yu Lu Cheng Sheng Dai Yongjun Jiang Bing Yang Hong Li Yi Zhao Jing Xu Ying Zhang Chengsi Pan Xiao‐Ming Cao Yongfa Zhu Yang Lou |
| author_facet | Baiyang Yu Lu Cheng Sheng Dai Yongjun Jiang Bing Yang Hong Li Yi Zhao Jing Xu Ying Zhang Chengsi Pan Xiao‐Ming Cao Yongfa Zhu Yang Lou |
| author_sort | Baiyang Yu |
| collection | DOAJ |
| description | Abstract Rationally constructing atom‐precise active sites is highly important to promote their catalytic performance but still challenging. Herein, this work designs and constructs ZSM‐5 supported Cu and Ag dual single atoms as a proof‐of‐concept catalyst (Ag1−Cu1/ZSM‐5 hetero‐SAC (single‐atom catalyst)) to boost direct oxidation of methane (DOM) by H2O2. The Ag1−Cu1/ZSM‐5 hetero‐SAC synthesized via a modified co‐adsorption strategy yields a methanol productivity of 20,115 µmol gcat−1 with 81% selectivity at 70 °C within 30 min, which surpasses most of the state‐of‐the‐art noble metal catalysts. The characterization results prove that the synergistic interaction between silver and copper facilitates the formation of highly reactive surface hydroxyl species to activate the C−H bond as well as the activity, selectivity, and stability of DOM compared with SACs, which is the key to the enhanced catalytic performance. This work believes the atomic‐level design strategy on dual‐single‐atom active sites should pave the way to designing advanced catalysts for methane conversion. |
| first_indexed | 2024-03-12T00:37:31Z |
| format | Article |
| id | doaj.art-c71fe598070a4d4eb75e950d74d9ea79 |
| institution | Directory Open Access Journal |
| issn | 2198-3844 |
| language | English |
| last_indexed | 2024-03-12T00:37:31Z |
| publishDate | 2023-09-01 |
| publisher | Wiley |
| record_format | Article |
| series | Advanced Science |
| spelling | doaj.art-c71fe598070a4d4eb75e950d74d9ea792023-09-15T09:28:59ZengWileyAdvanced Science2198-38442023-09-011026n/an/a10.1002/advs.202302143Silver and Copper Dual Single Atoms Boosting Direct Oxidation of Methane to Methanol via Synergistic CatalysisBaiyang Yu0Lu Cheng1Sheng Dai2Yongjun Jiang3Bing Yang4Hong Li5Yi Zhao6Jing Xu7Ying Zhang8Chengsi Pan9Xiao‐Ming Cao10Yongfa Zhu11Yang Lou12Key Laboratory of Synthetic and Biological Colloids, Ministry of Education, School of Chemical and Material Engineering Jiangnan University Wuxi Jiangsu 214122 ChinaKey Laboratory for Advanced Materials and Feringa Nobel Prize Scientist Joint Research Center, School of Chemistry and Molecular Engineering East China University of Science and Technology Shanghai 200237 ChinaKey Laboratory for Advanced Materials and Feringa Nobel Prize Scientist Joint Research Center, School of Chemistry and Molecular Engineering East China University of Science and Technology Shanghai 200237 ChinaKey Laboratory for Advanced Materials and Feringa Nobel Prize Scientist Joint Research Center, School of Chemistry and Molecular Engineering East China University of Science and Technology Shanghai 200237 ChinaDalian National Laboratory for Clean Energy Dalian Institute of Chemical Physics 457 Zhongshan Road Dalian 116023 ChinaDalian National Laboratory for Clean Energy Dalian Institute of Chemical Physics 457 Zhongshan Road Dalian 116023 ChinaKey Laboratory of Synthetic and Biological Colloids, Ministry of Education, School of Chemical and Material Engineering Jiangnan University Wuxi Jiangsu 214122 ChinaSchool of Food Science and Technology Jiangnan University Wuxi Jiangsu 214122 ChinaKey Laboratory of Synthetic and Biological Colloids, Ministry of Education, School of Chemical and Material Engineering Jiangnan University Wuxi Jiangsu 214122 ChinaKey Laboratory of Synthetic and Biological Colloids, Ministry of Education, School of Chemical and Material Engineering Jiangnan University Wuxi Jiangsu 214122 ChinaKey Laboratory for Advanced Materials and Feringa Nobel Prize Scientist Joint Research Center, School of Chemistry and Molecular Engineering East China University of Science and Technology Shanghai 200237 ChinaDepartment of Chemistry Tsinghua University Beijing 100084 ChinaKey Laboratory of Synthetic and Biological Colloids, Ministry of Education, School of Chemical and Material Engineering Jiangnan University Wuxi Jiangsu 214122 ChinaAbstract Rationally constructing atom‐precise active sites is highly important to promote their catalytic performance but still challenging. Herein, this work designs and constructs ZSM‐5 supported Cu and Ag dual single atoms as a proof‐of‐concept catalyst (Ag1−Cu1/ZSM‐5 hetero‐SAC (single‐atom catalyst)) to boost direct oxidation of methane (DOM) by H2O2. The Ag1−Cu1/ZSM‐5 hetero‐SAC synthesized via a modified co‐adsorption strategy yields a methanol productivity of 20,115 µmol gcat−1 with 81% selectivity at 70 °C within 30 min, which surpasses most of the state‐of‐the‐art noble metal catalysts. The characterization results prove that the synergistic interaction between silver and copper facilitates the formation of highly reactive surface hydroxyl species to activate the C−H bond as well as the activity, selectivity, and stability of DOM compared with SACs, which is the key to the enhanced catalytic performance. This work believes the atomic‐level design strategy on dual‐single‐atom active sites should pave the way to designing advanced catalysts for methane conversion.https://doi.org/10.1002/advs.202302143dual‐atom centersmethane direct conversionmethanolselective conversionsynergistic catalysis |
| spellingShingle | Baiyang Yu Lu Cheng Sheng Dai Yongjun Jiang Bing Yang Hong Li Yi Zhao Jing Xu Ying Zhang Chengsi Pan Xiao‐Ming Cao Yongfa Zhu Yang Lou Silver and Copper Dual Single Atoms Boosting Direct Oxidation of Methane to Methanol via Synergistic Catalysis Advanced Science dual‐atom centers methane direct conversion methanol selective conversion synergistic catalysis |
| title | Silver and Copper Dual Single Atoms Boosting Direct Oxidation of Methane to Methanol via Synergistic Catalysis |
| title_full | Silver and Copper Dual Single Atoms Boosting Direct Oxidation of Methane to Methanol via Synergistic Catalysis |
| title_fullStr | Silver and Copper Dual Single Atoms Boosting Direct Oxidation of Methane to Methanol via Synergistic Catalysis |
| title_full_unstemmed | Silver and Copper Dual Single Atoms Boosting Direct Oxidation of Methane to Methanol via Synergistic Catalysis |
| title_short | Silver and Copper Dual Single Atoms Boosting Direct Oxidation of Methane to Methanol via Synergistic Catalysis |
| title_sort | silver and copper dual single atoms boosting direct oxidation of methane to methanol via synergistic catalysis |
| topic | dual‐atom centers methane direct conversion methanol selective conversion synergistic catalysis |
| url | https://doi.org/10.1002/advs.202302143 |
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