Quantifying the distinct role of plasmon enhancement mechanisms in prototypical antenna-reactor photocatalysts
Abstract Plasmonic photocatalysis enabled by the unique localized surface plasmon resonance represents a promising approach for efficient solar energy conversion. Elucidating the distinct plasmonic catalytic mechanisms and quantification of their effect is crucial yet highly challenging, due to thei...
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Nature Portfolio
2025-03-01
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| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-025-57569-0 |
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| author | Shuang Liu Zhiyi Wu Zhijie Zhu Kai Feng Yuxuan Zhou Xinge Hu Xiong Huang Binbin Zhang Xudong Dong Yueru Ma Kaiqi Nie Jiahui Shen Zidi Wang Jiari He Jiaqi Wang Yu Ji Binhang Yan Qingfeng Zhang Alexander Genest Xiaohong Zhang Chaoran Li Bo Wu Xingda An Günther Rupprechter Le He |
| author_facet | Shuang Liu Zhiyi Wu Zhijie Zhu Kai Feng Yuxuan Zhou Xinge Hu Xiong Huang Binbin Zhang Xudong Dong Yueru Ma Kaiqi Nie Jiahui Shen Zidi Wang Jiari He Jiaqi Wang Yu Ji Binhang Yan Qingfeng Zhang Alexander Genest Xiaohong Zhang Chaoran Li Bo Wu Xingda An Günther Rupprechter Le He |
| author_sort | Shuang Liu |
| collection | DOAJ |
| description | Abstract Plasmonic photocatalysis enabled by the unique localized surface plasmon resonance represents a promising approach for efficient solar energy conversion. Elucidating the distinct plasmonic catalytic mechanisms and quantification of their effect is crucial yet highly challenging, due to their complex and synergistic nature. Herein, we achieve the differentiation and quantification of thermal as well as various non-thermal reaction mechanisms in prototypical Au-[Fe(bpy)3]2+ antenna-reactor photocatalysts using water splitting as test reaction. Through modification of the resonance condition and connection schemes, non-thermal plasmonic charge and energy transfer mechanisms are selectively shielded. It is found that plasmonic charge carrier-induced photochemistry dominates the photocurrent (~57%) in a reducing, hydrogen evolution environment; whereas resonant plasmonic energy transfer dominates (~54%) in an oxidative, oxygen evolution environment. Our approach provides generalized and fundamental understandings on the role of surface plasmons in photocatalysis as well as important design principles for plasmonic photocatalysts towards distinct reaction types and catalyst configurations. |
| format | Article |
| id | doaj-art-88da693e9cf14e4a9236c8453db63f79 |
| institution | OA Journals |
| issn | 2041-1723 |
| language | English |
| publishDate | 2025-03-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Nature Communications |
| spelling | doaj-art-88da693e9cf14e4a9236c8453db63f792025-08-20T02:16:06ZengNature PortfolioNature Communications2041-17232025-03-0116111210.1038/s41467-025-57569-0Quantifying the distinct role of plasmon enhancement mechanisms in prototypical antenna-reactor photocatalystsShuang Liu0Zhiyi Wu1Zhijie Zhu2Kai Feng3Yuxuan Zhou4Xinge Hu5Xiong Huang6Binbin Zhang7Xudong Dong8Yueru Ma9Kaiqi Nie10Jiahui Shen11Zidi Wang12Jiari He13Jiaqi Wang14Yu Ji15Binhang Yan16Qingfeng Zhang17Alexander Genest18Xiaohong Zhang19Chaoran Li20Bo Wu21Xingda An22Günther Rupprechter23Le He24Institute of Functional Nano & Soft Materials (FUNSOM) and Jiangsu Key Laboratory of Advanced Negative Carbon Technologies, Soochow UniversityInstitute of Functional Nano & Soft Materials (FUNSOM) and Jiangsu Key Laboratory of Advanced Negative Carbon Technologies, Soochow UniversityInstitute of Functional Nano & Soft Materials (FUNSOM) and Jiangsu Key Laboratory of Advanced Negative Carbon Technologies, Soochow UniversityInstitute of Functional Nano & Soft Materials (FUNSOM) and Jiangsu Key Laboratory of Advanced Negative Carbon Technologies, Soochow UniversityInstitute of Functional Nano & Soft Materials (FUNSOM) and Jiangsu Key Laboratory of Advanced Negative Carbon Technologies, Soochow UniversityInstitute of Functional Nano & Soft Materials (FUNSOM) and Jiangsu Key Laboratory of Advanced Negative Carbon Technologies, Soochow UniversityGuangdong Provincial Key Laboratory of Optical Information Materials and Technology, Institute of Electronic Paper Displays, South China Academy of Advanced Optoelectronics, South China Normal UniversityCollege of Chemistry and Molecular Sciences, Wuhan UniversityInstitute of Functional Nano & Soft Materials (FUNSOM) and Jiangsu Key Laboratory of Advanced Negative Carbon Technologies, Soochow UniversityInstitute of Functional Nano & Soft Materials (FUNSOM) and Jiangsu Key Laboratory of Advanced Negative Carbon Technologies, Soochow UniversityDepartment of Chemical Engineering, Tsinghua UniversityInstitute of Functional Nano & Soft Materials (FUNSOM) and Jiangsu Key Laboratory of Advanced Negative Carbon Technologies, Soochow UniversityInstitute of Functional Nano & Soft Materials (FUNSOM) and Jiangsu Key Laboratory of Advanced Negative Carbon Technologies, Soochow UniversityState Key Laboratory of Crystal Materials, Institute of Crystal Materials, Shandong UniversityInstitute of Functional Nano & Soft Materials (FUNSOM) and Jiangsu Key Laboratory of Advanced Negative Carbon Technologies, Soochow UniversityInstitute of Functional Nano & Soft Materials (FUNSOM) and Jiangsu Key Laboratory of Advanced Negative Carbon Technologies, Soochow UniversityDepartment of Chemical Engineering, Tsinghua UniversityCollege of Chemistry and Molecular Sciences, Wuhan UniversityInstitute of Materials Chemistry, TU WienInstitute of Functional Nano & Soft Materials (FUNSOM) and Jiangsu Key Laboratory of Advanced Negative Carbon Technologies, Soochow UniversityInstitute of Functional Nano & Soft Materials (FUNSOM) and Jiangsu Key Laboratory of Advanced Negative Carbon Technologies, Soochow UniversityGuangdong Provincial Key Laboratory of Optical Information Materials and Technology, Institute of Electronic Paper Displays, South China Academy of Advanced Optoelectronics, South China Normal UniversityInstitute of Functional Nano & Soft Materials (FUNSOM) and Jiangsu Key Laboratory of Advanced Negative Carbon Technologies, Soochow UniversityInstitute of Materials Chemistry, TU WienInstitute of Functional Nano & Soft Materials (FUNSOM) and Jiangsu Key Laboratory of Advanced Negative Carbon Technologies, Soochow UniversityAbstract Plasmonic photocatalysis enabled by the unique localized surface plasmon resonance represents a promising approach for efficient solar energy conversion. Elucidating the distinct plasmonic catalytic mechanisms and quantification of their effect is crucial yet highly challenging, due to their complex and synergistic nature. Herein, we achieve the differentiation and quantification of thermal as well as various non-thermal reaction mechanisms in prototypical Au-[Fe(bpy)3]2+ antenna-reactor photocatalysts using water splitting as test reaction. Through modification of the resonance condition and connection schemes, non-thermal plasmonic charge and energy transfer mechanisms are selectively shielded. It is found that plasmonic charge carrier-induced photochemistry dominates the photocurrent (~57%) in a reducing, hydrogen evolution environment; whereas resonant plasmonic energy transfer dominates (~54%) in an oxidative, oxygen evolution environment. Our approach provides generalized and fundamental understandings on the role of surface plasmons in photocatalysis as well as important design principles for plasmonic photocatalysts towards distinct reaction types and catalyst configurations.https://doi.org/10.1038/s41467-025-57569-0 |
| spellingShingle | Shuang Liu Zhiyi Wu Zhijie Zhu Kai Feng Yuxuan Zhou Xinge Hu Xiong Huang Binbin Zhang Xudong Dong Yueru Ma Kaiqi Nie Jiahui Shen Zidi Wang Jiari He Jiaqi Wang Yu Ji Binhang Yan Qingfeng Zhang Alexander Genest Xiaohong Zhang Chaoran Li Bo Wu Xingda An Günther Rupprechter Le He Quantifying the distinct role of plasmon enhancement mechanisms in prototypical antenna-reactor photocatalysts Nature Communications |
| title | Quantifying the distinct role of plasmon enhancement mechanisms in prototypical antenna-reactor photocatalysts |
| title_full | Quantifying the distinct role of plasmon enhancement mechanisms in prototypical antenna-reactor photocatalysts |
| title_fullStr | Quantifying the distinct role of plasmon enhancement mechanisms in prototypical antenna-reactor photocatalysts |
| title_full_unstemmed | Quantifying the distinct role of plasmon enhancement mechanisms in prototypical antenna-reactor photocatalysts |
| title_short | Quantifying the distinct role of plasmon enhancement mechanisms in prototypical antenna-reactor photocatalysts |
| title_sort | quantifying the distinct role of plasmon enhancement mechanisms in prototypical antenna reactor photocatalysts |
| url | https://doi.org/10.1038/s41467-025-57569-0 |
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