Enhanced hydrogen peroxide photosynthesis via charge-complementary π-electron sites

Yan Guo, Qixin Zhou, Li Wang, Ziqi Deng, David Lee Phillips, Chuyang Y. Tang () and Yongfa Zhu ()
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Yan Guo: The University of Hong Kong
Qixin Zhou: Tsinghua University
Li Wang: The University of Hong Kong
Ziqi Deng: The University of Hong Kong
David Lee Phillips: The University of Hong Kong
Chuyang Y. Tang: The University of Hong Kong
Yongfa Zhu: Tsinghua University

Nature Communications, 2025, vol. 16, issue 1, 1-11

Abstract: Abstract Organic photocatalysts with porphyrin conjugated chromophore core are promising for artificial hydrogen peroxide (H2O2) photosynthesis, but the lack of bottom-up paradigm for oxygen (O2) adsorption sites hinders their activity. Here, we introduce imidazole groups as π-electron sites with charge-complementarity to the O2 molecules, enhancing O2 binding via sub-atomically mirrored electrostatic cooperative π-π dispersion forces. In situ spectroscopy and theory reveal that the ~2 Å linear δ+-δ−-δ+ domain of the imidazole substituent exhibits 2.8-folds stronger O2 adsorption than neutral π-electron substituents, accompanied by the generation of energetically peroxide intermediates. Consequently, imidazole-substituted porphyrin photocatalysts achieve a solar-to-chemical conversion efficiency of 1.85% using only H2O and O2. In scalable membranes with photocatalysts, enabling daily photosynthetic production of 80 L m−2 of Fenton-applicable H2O2 solution. This work offers a strategy to modulate the electrostatic distribution of oxygen photoreduction sites, providing insights into overcoming gas activation rate-limiting steps in photocatalytic processes.

Date: 2025
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DOI: 10.1038/s41467-025-61452-3

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