Authors
Danfeng Wang, Heman Xu, Yihan Tang, Lixuan Kan, Jingwen Dong, Shiyuan Zhou, Qianfeng Gu, Yuzhe Zhang, Guangfeng Liu, Qichun Zhang, Peiyang Gu
Published in
Angewandte Chemie (International ed. in English). Pages e6174836. Sep 08, 2026. Epub Sep 08, 2026.
Abstract
Maximizing photon utilization in organic photocatalysis requires harnessing both singlet and triplet excitons, however, the strategies to populate the spin-forbidden triplet state in metal-free polymers are rare. To address this issue, we report a new strategy, namely employing a spin-orbit charge transfer intersystem crossing (SOCT-ISC), to unlock the triplet manifold in conjugated microporous polymers (CMPs). Using a postsynthetic [2 + 2] cycloaddition-retroelectrocyclization (CA-RE) reaction, we precisely control the cyano number in the polymer backbone. This chemical modification induces a critical orthogonal molecular torsion, which maximizes spin-orbit coupling (SOC) and minimizes the singlet-triplet energy gap (ΔEST). Femtosecond transient absorption spectroscopy confirms the efficient triplet generation by torsion engineering. Consequently, the optimized photocatalyst achieves a hydrogen peroxide (H2O2) production rate of 5.01 mmol g-1 h-1 in pure water and a rate of 101.26 mmol g-1 h-1 in a benzyl alcohol-coupled system, with a solar-to-chemical conversion (SCC) efficiency of 0.62%, and an outdoor production reaches 5 mmol L-1 daily. This work leverages torsion engineering to harness triplet excitons, demonstrating the successful overcoming of thermodynamic barriers in artificial photosynthesis.
PMID:
42711705
Bibliographic data and abstract were imported from PubMed on 09 Sep 2026.
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