Stabilizing the excited states of organic phosphorescent photosensitizers via self-assembly for CO<sub>2</sub> photoreduction.
basic_science · Level V
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- Record sourced from PubMed, PMID 40610510.
- Also identified by DOI 10.1038/s41467-025-61451-4 and PMC identifier 12229595.
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Abstract
The development of pure organic photosensitizers remains challenging due to the low intersystem crossing efficiency and the instability of triplet excitons. Herein, fused-ring phosphorescent molecules enhance visible-light absorption, with heteroatom-rich structures breaking the restriction of low triplet excitons. A derivative, 2,3,5,6,9,10-hexabutoxy-8-phenyldithieno-tribenzo-pyridine (TPy), exhibits high ISC efficiency and efficiently sensitizes Fe-catalysts for CO<sub>2</sub> photoreduction to CO. We further developed a self-assembly method to stabilize triplet excitons by embedding TPy within the rigid core of amphiphilic polymer nanoparticles. The hydrophobic core of the nanoparticles significantly prolongs the excited-state lifetime, while the hydrophilic shell ensures excellent dispersibility and stability. This system achieves a turnover number of 2041 and retains 93.5% of its initial activity after three cycles. Our work provides a general strategy for designing stable and highly efficient organic photosensitizers, paving the way for sustainable photoredox catalysis.