Stabilizing the excited states of organic phosphorescent photosensitizers via self-assembly for CO2 photoreduction

Chenchen Xiong, Ping Wang, Yao Ma, Yongfeng Zhang, Xin Cheng, Cong Chao, Lingling Kang, Gengchen Li, Peng Sun, Jianbing Shi, Bin Tong, Xiangfeng Shao (), Zhi-Ming Zhang (), Zhengxu Cai () and Yuping Dong
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Chenchen Xiong: Beijing Institute of Technology
Ping Wang: Tianjin University of Technology
Yao Ma: Tianshui Southern Road 222
Yongfeng Zhang: Beijing Institute of Technology
Xin Cheng: Beijing Institute of Technology
Cong Chao: North China Electric Power University
Lingling Kang: Beijing Institute of Technology
Gengchen Li: Beijing Institute of Technology
Peng Sun: Beijing Institute of Technology
Jianbing Shi: Beijing Institute of Technology
Bin Tong: Beijing Institute of Technology
Xiangfeng Shao: Tianshui Southern Road 222
Zhi-Ming Zhang: Tianjin University of Technology
Zhengxu Cai: Beijing Institute of Technology
Yuping Dong: Beijing Institute of Technology

Nature Communications, 2025, vol. 16, issue 1, 1-10

Abstract: 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 CO2 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.

Date: 2025
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DOI: 10.1038/s41467-025-61451-4

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