Steering artificial photosynthesis via photoinduced conversion of monometallic to bimetallic sites in FeCo nitroprussides

Hao Wang, Gui-Lin Zhuang, Yingjie Fan, Hua-Qing Yin (), Wei Zhang, Zhe Wu, Shuang Yao, Tong-Bu Lu, Wenbin Lin () and Zhi-Ming Zhang ()
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Hao Wang: Tianjin University of Technology
Gui-Lin Zhuang: Zhejiang University of Technology
Yingjie Fan: The University of Chicago
Hua-Qing Yin: Tianjin University of Technology
Wei Zhang: Zhejiang University of Technology
Zhe Wu: Tianjin University of Technology
Shuang Yao: Tianjin University of Technology
Tong-Bu Lu: Tianjin University of Technology
Wenbin Lin: The University of Chicago
Zhi-Ming Zhang: Tianjin University of Technology

Nature Communications, 2025, vol. 16, issue 1, 1-13

Abstract: Abstract Artificial photosynthesis provides an efficient strategy for solar energy storage via water splitting and CO2 reduction, but it remains a challenge in tuning artificial photosynthesis between these two competing reactions. Herein, we demonstrate photoinduced conversion of monometallic to bimetallic sites in a Fe-Co nitroprusside (FeCo–NP) to steer the reaction path from H2 evolution to CO2 reduction. Monometallic Co sites achieve efficient H2 production with 28.5 mmol g−1 activity and 85.4% selectivity. Photoinduced release of nitrosyl groups from Fe sites generates bimetallic Fe-Co sites, which suppress H2 evolution and enhance CO2 reduction, yielding 31.5 mmol g−1 activity and 87.3% selectivity for C1 products. Mechanistic investigations reveal that monometallic Co sites catalyze H2 evolution via H2O adsorption and O-H cleavage while bimetallic Fe-Co sites facilitate both H2O and CO2 adsorption and subsequent O and C hydrogenation for CO and HCOOH. This work uncovers a strategy to manipulate competing reaction pathways via photoinduced conversion of monometallic to bimetallic sites, which provides unique insights into addressing environmental issues and energy crises.

Date: 2025
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DOI: 10.1038/s41467-025-61129-x

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