Dynamic Valence-State-Adaptive Ta Single-Atom Sites for Artificial H <sub>2</sub> O <sub>2</sub> Photosynthesis

Photocatalytic H 2 O 2 synthesis via the two-electron O 2 reduction reaction (2e – ORR) is attractive, yet the interplay between active-site-mediated excited-state electron behavior and in situ O 2 activation at the atomic scale remains unclear. Herein, we establish a mechanism-guided integrated strategy combining theoretical screening, experimental construction, and in situ characterization to identify Ta single-atom sites as the optimal 5d metal centers on carbon nitride for H 2 O 2 photosynthesis. The resulting catalyst combines favorable excited-state charge localization with thermodynamic advantages for the 2e – ORR, achieving an apparent quantum yield of 14.53% at 420 nm and a solar-to-chemical conversion efficiency of 1.12% in pure water. Multidimensional in situ spectroscopy measurements and theoretical calculations demonstrate that Ta single-atom sites act as dynamically adaptive catalytic centers through flexible in situ valence-state evolution (+4.16 → +4.37 → +3.14), facilitating initial O 2 adsorption and then accumulating and transferring excited-state electrons to drive end-on O 2 activation through Ta 5d-O 2p orbital coupling, thereby accelerating *OOH-mediated selective H 2 O 2 formation. This work establishes a framework for understanding dynamic single-atom photocatalysis and guiding the design of adaptive active sites for artificial H 2 O 2 photosynthesis.

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Publication Details

Journal
Journal of the American Chemical Society
Published
2026-06-30
DOI
https://doi.org/10.1021/jacs.6c09675
Primary Topic
Advanced Photocatalysis Techniques
Type
article
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article

Dynamic Valence-State-Adaptive Ta Single-Atom Sites for Artificial H 2 O 2 Photosynthesis

Hanwen Hu, X Xiuzhen Feng, Laiyu Luo, Yueshuai Wang et al.
Journal of the American Chemical Society
Advanced Photocatalysis Techniques
article

Dynamic Valence-State-Adaptive Ta Single-Atom Sites for Artificial H 2 O 2 Photosynthesis

Hanwen Hu, X Xiuzhen Feng, Laiyu Luo, Yueshuai Wang, Tierui Zhang, Qixin Zhou, Shuowen Bo, Caoyu Yang, Chenliang Su, Bin Liu, Qinghua Liu, Xi Zhang, Jie Ding, Kun Zheng, Lingyue Liu, J Z Zhao, Yi-Xiang Wang, C R Yang, Taoran Chen, Bing Wang, Ying Tao, Hongli Sun
article en

Abstract

Photocatalytic H 2 O 2 synthesis via the two-electron O 2 reduction reaction (2e – ORR) is attractive, yet the interplay between active-site-mediated excited-state electron behavior and in situ O 2 activation at the atomic scale remains unclear. Herein, we establish a mechanism-guided integrated strategy combining theoretical screening, experimental construction, and in situ characterization to identify Ta single-atom sites as the optimal 5d metal centers on carbon nitride for H 2 O 2 photosynthesis. The resulting catalyst combines favorable excited-state charge localization with thermodynamic advantages for the 2e – ORR, achieving an apparent quantum yield of 14.53% at 420 nm and a solar-to-chemical conversion efficiency of 1.12% in pure water. Multidimensional in situ spectroscopy measurements and theoretical calculations demonstrate that Ta single-atom sites act as dynamically adaptive catalytic centers through flexible in situ valence-state evolution (+4.16 → +4.37 → +3.14), facilitating initial O 2 adsorption and then accumulating and transferring excited-state electrons to drive end-on O 2 activation through Ta 5d-O 2p orbital coupling, thereby accelerating *OOH-mediated selective H 2 O 2 formation. This work establishes a framework for understanding dynamic single-atom photocatalysis and guiding the design of adaptive active sites for artificial H 2 O 2 photosynthesis.

Journal of the American Chemical Society
University of Science and Technology of China (CN), City University of Hong Kong (HK), Shenzhen University (CN), Chinese Academy of Sciences (CN), Center for NanoScience (DE), Beijing University of Technology (CN), Crystal Research (United States) (US), Nanosystem (Russia) (RU), Division of Materials Science and Engineering (AU), Microscale (United States) (US), Technical Institute of Physics and Chemistry (CN), National Center for Nanoscience and Technology (CN), Advanced Materials and Devices (United States) (US), National Synchrotron Radiation Laboratory (CN), Xijing University (CN), East China Normal University (CN)
Clean water and sanitation
Openalex Percentile: Top 20%
Advanced Photocatalysis Techniques
DOISourceOpenAlex
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