作者：

Shuang Liu^1#, Zhiyi Wu^1#, Zhijie Zhu^1#, Kai Feng¹, Yuxuan Zhou¹, Xinge Hu¹, Xiong Huang², Binbin Zhang³, Xudong Dong¹, Yueru Ma¹, Kaiqi Nie⁴, Jiahui Shen¹, Zidi Wang¹, Jiari He⁵, Jiaqi Wang¹, Yu Ji¹, Binhang Yan⁴, Qingfeng Zhang³, Alexander Genest⁶, Xiaohong Zhang¹, Chaoran Li^{1, 7}*, Bo Wu², Xingda An¹*, Günther Rupprechter⁶ & Le He¹*

摘要：

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.

影响因子：

14.7

分区情况：

一区