Electron-Deficient Zn-N6 Configuration Enabling Polymeric Carbon Nitride for Visible-Light Photocatalytic Overall Water Splitting
Abstract Despite of suitable band structures for harvesting solar light and driving water redox reactions, polymeric carbon nitride (PCN) has suffered from poor charge transfer ability and sluggish surface reaction kinetics, which limit its photocatalytic activity for water splitting. Herein, atomic...
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| Format: | Article |
| Language: | English |
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SpringerOpen
2022-11-01
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| Series: | Nano-Micro Letters |
| Subjects: | |
| Online Access: | https://doi.org/10.1007/s40820-022-00962-x |
| _version_ | 1828127852945473536 |
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| author | Daming Zhao Yiqing Wang Chung-Li Dong Fanqi Meng Yu-Cheng Huang Qinghua Zhang Lin Gu Lan Liu Shaohua Shen |
| author_facet | Daming Zhao Yiqing Wang Chung-Li Dong Fanqi Meng Yu-Cheng Huang Qinghua Zhang Lin Gu Lan Liu Shaohua Shen |
| author_sort | Daming Zhao |
| collection | DOAJ |
| description | Abstract Despite of suitable band structures for harvesting solar light and driving water redox reactions, polymeric carbon nitride (PCN) has suffered from poor charge transfer ability and sluggish surface reaction kinetics, which limit its photocatalytic activity for water splitting. Herein, atomically dispersed Zn-coordinated three-dimensional (3D) sponge-like PCN (Zn-PCN) is synthesized through a novel intermediate coordination strategy. Advanced characterizations and theoretical calculations well evidence that Zn single atoms are coordinated and stabilized on PCN in the form of Zn-N6 configuration featured with an electron-deficient state. Such an electronic configuration has been demonstrated contributive to promoted electron excitation, accelerated charge separation and transfer as well as reduced water redox barriers. Further benefited from the abundant surface active sites derived from the 3D porous structure, Zn-PCN realizes visible-light photocatalysis for overall water splitting with H2 and O2 simultaneously evolved at a stoichiometric ratio of 2:1. This work brings new insights into the design of novel single-atom photocatalysts by deepening the understanding of electronic configurations and reactive sites favorable to excellent photocatalysis for water splitting and related solar energy conversion reactions. |
| first_indexed | 2024-04-11T15:55:55Z |
| format | Article |
| id | doaj.art-a0d0c15259584d12a73646747c4dba5c |
| institution | Directory Open Access Journal |
| issn | 2311-6706 2150-5551 |
| language | English |
| last_indexed | 2024-04-11T15:55:55Z |
| publishDate | 2022-11-01 |
| publisher | SpringerOpen |
| record_format | Article |
| series | Nano-Micro Letters |
| spelling | doaj.art-a0d0c15259584d12a73646747c4dba5c2022-12-22T04:15:10ZengSpringerOpenNano-Micro Letters2311-67062150-55512022-11-0114111510.1007/s40820-022-00962-xElectron-Deficient Zn-N6 Configuration Enabling Polymeric Carbon Nitride for Visible-Light Photocatalytic Overall Water SplittingDaming Zhao0Yiqing Wang1Chung-Li Dong2Fanqi Meng3Yu-Cheng Huang4Qinghua Zhang5Lin Gu6Lan Liu7Shaohua Shen8International Research Center for Renewable Energy, State Key Laboratory of Multiphase Flow in Power Engineering, Xi’an Jiaotong UniversityInternational Research Center for Renewable Energy, State Key Laboratory of Multiphase Flow in Power Engineering, Xi’an Jiaotong UniversityDepartment of Physics, Tamkang UniversityBeijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of SciencesDepartment of Physics, Tamkang UniversityBeijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of SciencesBeijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of SciencesInternational Research Center for Renewable Energy, State Key Laboratory of Multiphase Flow in Power Engineering, Xi’an Jiaotong UniversityInternational Research Center for Renewable Energy, State Key Laboratory of Multiphase Flow in Power Engineering, Xi’an Jiaotong UniversityAbstract Despite of suitable band structures for harvesting solar light and driving water redox reactions, polymeric carbon nitride (PCN) has suffered from poor charge transfer ability and sluggish surface reaction kinetics, which limit its photocatalytic activity for water splitting. Herein, atomically dispersed Zn-coordinated three-dimensional (3D) sponge-like PCN (Zn-PCN) is synthesized through a novel intermediate coordination strategy. Advanced characterizations and theoretical calculations well evidence that Zn single atoms are coordinated and stabilized on PCN in the form of Zn-N6 configuration featured with an electron-deficient state. Such an electronic configuration has been demonstrated contributive to promoted electron excitation, accelerated charge separation and transfer as well as reduced water redox barriers. Further benefited from the abundant surface active sites derived from the 3D porous structure, Zn-PCN realizes visible-light photocatalysis for overall water splitting with H2 and O2 simultaneously evolved at a stoichiometric ratio of 2:1. This work brings new insights into the design of novel single-atom photocatalysts by deepening the understanding of electronic configurations and reactive sites favorable to excellent photocatalysis for water splitting and related solar energy conversion reactions.https://doi.org/10.1007/s40820-022-00962-xZn single atomsPolymeric carbon nitrideOverall water splittingPhotocatalysis |
| spellingShingle | Daming Zhao Yiqing Wang Chung-Li Dong Fanqi Meng Yu-Cheng Huang Qinghua Zhang Lin Gu Lan Liu Shaohua Shen Electron-Deficient Zn-N6 Configuration Enabling Polymeric Carbon Nitride for Visible-Light Photocatalytic Overall Water Splitting Nano-Micro Letters Zn single atoms Polymeric carbon nitride Overall water splitting Photocatalysis |
| title | Electron-Deficient Zn-N6 Configuration Enabling Polymeric Carbon Nitride for Visible-Light Photocatalytic Overall Water Splitting |
| title_full | Electron-Deficient Zn-N6 Configuration Enabling Polymeric Carbon Nitride for Visible-Light Photocatalytic Overall Water Splitting |
| title_fullStr | Electron-Deficient Zn-N6 Configuration Enabling Polymeric Carbon Nitride for Visible-Light Photocatalytic Overall Water Splitting |
| title_full_unstemmed | Electron-Deficient Zn-N6 Configuration Enabling Polymeric Carbon Nitride for Visible-Light Photocatalytic Overall Water Splitting |
| title_short | Electron-Deficient Zn-N6 Configuration Enabling Polymeric Carbon Nitride for Visible-Light Photocatalytic Overall Water Splitting |
| title_sort | electron deficient zn n6 configuration enabling polymeric carbon nitride for visible light photocatalytic overall water splitting |
| topic | Zn single atoms Polymeric carbon nitride Overall water splitting Photocatalysis |
| url | https://doi.org/10.1007/s40820-022-00962-x |
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