Authors
Haishan Zhu, Yihong Zhang, Yijin Wang, Chunqiang Zhuang, Junfeng Gao, Xuanhua Li
Published in
Advanced materials (Deerfield Beach, Fla.). Pages e75402. Oct 13, 2026. Epub Oct 13, 2026.
Abstract
Decoupling photocatalytic solar fuel generation from continuous illumination is a prerequisite for practical off-grid applications, yet demands precise control over photogenerated charge retention and dark-phase utilization. While persistent charge availability post-light cutoff is central to dark-state catalysis, a quantitative structure-dynamics-function relationship linking molecular design to charge-retention kinetics and post-illumination reactivity remains unestablished. Here, we report a molecular tuning strategy of the central amine-derived units that systematically regulates charge separation, retention timescales, and dark-state H2O2 production in imine-linked polymer networks. Systematic evaluation of the series reveals a direct correlation between charge lifetime and dark activity. Compared with the N-centered reference, the C3N3-centered analogue exhibits drastically prolonged electron-associated transient lifetime, with a ∼27-fold longer decay timescale at the picosecond scale and a ∼3-fold increase at the nanosecond scale. This enhanced charge retention corresponds to a dark-state H2O2 production of 4941 µmol g-1 within 40 min, ∼1.5-fold higher than that of the N-centered counterpart. Density functional theory calculations reveal distinct electronic structures associated within the C3N3-centered framework, providing a favorable electronic environment for electron localization and subsequent utilization. These results establish a molecular structure-charge retention-dark reaction relationship for photocatalytic H2O2 production beyond the illumination period.
PMID:
42865323
Bibliographic data and abstract were imported from PubMed on 13 Oct 2026.
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