Quantifying the distinct role of plasmon enhancement mechanisms in prototypical antenna-reactor photocatalysts

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 and Le He ()
Additional contact information
Shuang Liu: Soochow University
Zhiyi Wu: Soochow University
Zhijie Zhu: Soochow University
Kai Feng: Soochow University
Yuxuan Zhou: Soochow University
Xinge Hu: Soochow University
Xiong Huang: South China Normal University
Binbin Zhang: Wuhan University
Xudong Dong: Soochow University
Yueru Ma: Soochow University
Kaiqi Nie: Tsinghua University
Jiahui Shen: Soochow University
Zidi Wang: Soochow University
Jiari He: Shandong University
Jiaqi Wang: Soochow University
Yu Ji: Soochow University
Binhang Yan: Tsinghua University
Qingfeng Zhang: Wuhan University
Alexander Genest: TU Wien
Xiaohong Zhang: Soochow University
Chaoran Li: Soochow University
Bo Wu: South China Normal University
Xingda An: Soochow University
Günther Rupprechter: TU Wien
Le He: Soochow University

Nature Communications, 2025, vol. 16, issue 1, 1-12

Abstract: 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.

Date: 2025
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DOI: 10.1038/s41467-025-57569-0

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