Asymmetric coordination enhances the synergy of Pt species dual active sites for efficient photocatalytic H2 evolution

Bo Li, Hongshun Zheng, Tong Zhou (), Qingjie Lu, Mingpeng Chen, Huachuan Sun, Yuxiao Zhang, Yumin Zhang, Dequan Li, Baoye Zi, Mao Zhang, Jin Zhang, Jianhong Zhao, Tianwei He, Zhongqi Zhu, Genlin Zhang and Qingju Liu ()
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Bo Li: Yunnan University
Hongshun Zheng: Yunnan University
Tong Zhou: Yunnan University
Qingjie Lu: Yunnan University
Mingpeng Chen: Yunnan University
Huachuan Sun: Yunnan University
Yuxiao Zhang: Yunnan University
Yumin Zhang: Yunnan University
Dequan Li: Yunnan University
Baoye Zi: Yunnan University
Mao Zhang: Yunnan University
Jin Zhang: Yunnan University
Jianhong Zhao: Yunnan University
Tianwei He: Yunnan University
Zhongqi Zhu: Yunnan University
Genlin Zhang: Yunnan University
Qingju Liu: Yunnan University

Nature Communications, 2025, vol. 16, issue 1, 1-15

Abstract: Abstract Integrating distinct functional reaction sites within a single photocatalyst offers a promising approach for enhancing the photocatalytic H2 evolution by water splitting. However, the synergy between the dual active sites is hindered by suboptimal electronic states arising from the uniform coordination environments. Here we demonstrate a strategy for enhancing the synergy between Pt single atoms and nanoparticles by modulating the coordination environment. The optimal boron doped catalyst with B-Pt-O asymmetric coordination achieves a H2 evolution rate of 627.6 mmol g-1h-1, with an apparent quantum efficiency of 98.4%. Experimental and theoretical analysis reveal that the asymmetric coordination structure redistributes the electron density of Pt cocatalysts, promoting charge carrier separation, optimizing the dissociation and adsorption-desorption of the intermediate H2O* and H* on the dual sites. The findings highlight the importance of asymmetric coordination facilitates the photogenerated carrier transfer and surface reactions for efficient photocatalytic H2 evolution.

Date: 2025
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DOI: 10.1038/s41467-025-63637-2

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