Large electronegativity differences between adjacent atomic sites activate and stabilize ZnIn2S4 for efficient photocatalytic overall water splitting
Abstract Photocatalytic overall water splitting into hydrogen and oxygen is desirable for long-term renewable, sustainable and clean fuel production on earth. Metal sulfides are considered as ideal hydrogen-evolved photocatalysts, but their component homogeneity and typical sulfur instability cause...
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| Format: | Article |
| Language: | English |
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Nature Portfolio
2024-01-01
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| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-024-44725-1 |
| _version_ | 1827388325740150784 |
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| author | Xu Xin Yuke Li Youzi Zhang Yijin Wang Xiao Chi Yanping Wei Caozheng Diao Jie Su Ruiling Wang Peng Guo Jiakang Yu Jia Zhang Ana Jorge Sobrido Maria-Magdalena Titirici Xuanhua Li |
| author_facet | Xu Xin Yuke Li Youzi Zhang Yijin Wang Xiao Chi Yanping Wei Caozheng Diao Jie Su Ruiling Wang Peng Guo Jiakang Yu Jia Zhang Ana Jorge Sobrido Maria-Magdalena Titirici Xuanhua Li |
| author_sort | Xu Xin |
| collection | DOAJ |
| description | Abstract Photocatalytic overall water splitting into hydrogen and oxygen is desirable for long-term renewable, sustainable and clean fuel production on earth. Metal sulfides are considered as ideal hydrogen-evolved photocatalysts, but their component homogeneity and typical sulfur instability cause an inert oxygen production, which remains a huge obstacle to overall water-splitting. Here, a distortion-evoked cation-site oxygen doping of ZnIn2S4 (D-O-ZIS) creates significant electronegativity differences between adjacent atomic sites, with S1 sites being electron-rich and S2 sites being electron-deficient in the local structure of S1–S2–O sites. The strong charge redistribution character activates stable oxygen reactions at S2 sites and avoids the common issue of sulfur instability in metal sulfide photocatalysis, while S1 sites favor the adsorption/desorption of hydrogen. Consequently, an overall water-splitting reaction has been realized in D-O-ZIS with a remarkable solar-to-hydrogen conversion efficiency of 0.57%, accompanying a ~ 91% retention rate after 120 h photocatalytic test. In this work, we inspire an universal design from electronegativity differences perspective to activate and stabilize metal sulfide photocatalysts for efficient overall water-splitting. |
| first_indexed | 2024-03-08T16:16:14Z |
| format | Article |
| id | doaj.art-51538302fe284ec7b7e18806753e4eea |
| institution | Directory Open Access Journal |
| issn | 2041-1723 |
| language | English |
| last_indexed | 2024-03-08T16:16:14Z |
| publishDate | 2024-01-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Nature Communications |
| spelling | doaj.art-51538302fe284ec7b7e18806753e4eea2024-01-07T12:33:01ZengNature PortfolioNature Communications2041-17232024-01-0115111210.1038/s41467-024-44725-1Large electronegativity differences between adjacent atomic sites activate and stabilize ZnIn2S4 for efficient photocatalytic overall water splittingXu Xin0Yuke Li1Youzi Zhang2Yijin Wang3Xiao Chi4Yanping Wei5Caozheng Diao6Jie Su7Ruiling Wang8Peng Guo9Jiakang Yu10Jia Zhang11Ana Jorge Sobrido12Maria-Magdalena Titirici13Xuanhua Li14State Key Laboratory of Solidification Processing, Center for Nano Energy Materials, School of Materials Science and Engineering, Northwestern Polytechnical UniversityInstitute of High Performance Computing (IHPC), Agency for Science, Technology and Research (A*STAR)State Key Laboratory of Solidification Processing, Center for Nano Energy Materials, School of Materials Science and Engineering, Northwestern Polytechnical UniversityState Key Laboratory of Solidification Processing, Center for Nano Energy Materials, School of Materials Science and Engineering, Northwestern Polytechnical UniversityDepartment of Physics, National University of SingaporeCollege of Science, Gansu Agricultural UniversitySingapore Synchrotron Light Source, National University of SingaporeCollege of Microelectronics, Xidian UniversityState Key Laboratory of Solidification Processing, Center for Nano Energy Materials, School of Materials Science and Engineering, Northwestern Polytechnical UniversityState Key Laboratory of Solidification Processing, Center for Nano Energy Materials, School of Materials Science and Engineering, Northwestern Polytechnical UniversityState Key Laboratory of Solidification Processing, Center for Nano Energy Materials, School of Materials Science and Engineering, Northwestern Polytechnical UniversityInstitute of High Performance Computing (IHPC), Agency for Science, Technology and Research (A*STAR)School of Engineering and Materials Science, Faculty of Science and Engineering, Queen Mary University of LondonDepartment of Chemical Engineering, Imperial College London, South Kensington CampusState Key Laboratory of Solidification Processing, Center for Nano Energy Materials, School of Materials Science and Engineering, Northwestern Polytechnical UniversityAbstract Photocatalytic overall water splitting into hydrogen and oxygen is desirable for long-term renewable, sustainable and clean fuel production on earth. Metal sulfides are considered as ideal hydrogen-evolved photocatalysts, but their component homogeneity and typical sulfur instability cause an inert oxygen production, which remains a huge obstacle to overall water-splitting. Here, a distortion-evoked cation-site oxygen doping of ZnIn2S4 (D-O-ZIS) creates significant electronegativity differences between adjacent atomic sites, with S1 sites being electron-rich and S2 sites being electron-deficient in the local structure of S1–S2–O sites. The strong charge redistribution character activates stable oxygen reactions at S2 sites and avoids the common issue of sulfur instability in metal sulfide photocatalysis, while S1 sites favor the adsorption/desorption of hydrogen. Consequently, an overall water-splitting reaction has been realized in D-O-ZIS with a remarkable solar-to-hydrogen conversion efficiency of 0.57%, accompanying a ~ 91% retention rate after 120 h photocatalytic test. In this work, we inspire an universal design from electronegativity differences perspective to activate and stabilize metal sulfide photocatalysts for efficient overall water-splitting.https://doi.org/10.1038/s41467-024-44725-1 |
| spellingShingle | Xu Xin Yuke Li Youzi Zhang Yijin Wang Xiao Chi Yanping Wei Caozheng Diao Jie Su Ruiling Wang Peng Guo Jiakang Yu Jia Zhang Ana Jorge Sobrido Maria-Magdalena Titirici Xuanhua Li Large electronegativity differences between adjacent atomic sites activate and stabilize ZnIn2S4 for efficient photocatalytic overall water splitting Nature Communications |
| title | Large electronegativity differences between adjacent atomic sites activate and stabilize ZnIn2S4 for efficient photocatalytic overall water splitting |
| title_full | Large electronegativity differences between adjacent atomic sites activate and stabilize ZnIn2S4 for efficient photocatalytic overall water splitting |
| title_fullStr | Large electronegativity differences between adjacent atomic sites activate and stabilize ZnIn2S4 for efficient photocatalytic overall water splitting |
| title_full_unstemmed | Large electronegativity differences between adjacent atomic sites activate and stabilize ZnIn2S4 for efficient photocatalytic overall water splitting |
| title_short | Large electronegativity differences between adjacent atomic sites activate and stabilize ZnIn2S4 for efficient photocatalytic overall water splitting |
| title_sort | large electronegativity differences between adjacent atomic sites activate and stabilize znin2s4 for efficient photocatalytic overall water splitting |
| url | https://doi.org/10.1038/s41467-024-44725-1 |
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