Fluorinated chlorin chromophores for red-light-driven CO2 reduction

The utilization of low-energy photons in light-driven reactions is an effective strategy for improving the efficiency of solar energy conversion. In nature, photosynthetic organisms use chlorophylls to harvest the red portion of sunlight, which ultimately drives the reduction of CO 2 . However, a mo...

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Bibliographic Details
Published in:Nature communications 2024-07, Vol.15 (1), p.5704-10, Article 5704
Main Authors: Yang, Shuang, Yuan, Huiqing, Guo, Kai, Wei, Zuting, Ming, Mei, Yi, Jinzhi, Jiang, Long, Han, Zhiji
Format: Article
Language:English
Subjects:
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639/638/77/888
Carbon dioxide
Carbon dioxide concentration
Catalysis
Chromophores
Energy conversion
Fluorination
Humanities and Social Sciences
Intermediates
Irradiation
Light
Light irradiation
multidisciplinary
Noble metals
Photons
Porphyrins
Radiation
Science
Science (multidisciplinary)
Solar energy
Solar energy conversion
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Summary:The utilization of low-energy photons in light-driven reactions is an effective strategy for improving the efficiency of solar energy conversion. In nature, photosynthetic organisms use chlorophylls to harvest the red portion of sunlight, which ultimately drives the reduction of CO 2 . However, a molecular system that mimics such function is extremely rare in non-noble-metal catalysis. Here we report a series of synthetic fluorinated chlorins as biomimetic chromophores for CO 2 reduction, which catalytically produces CO under both 630 nm and 730 nm light irradiation, with turnover numbers of 1790 and 510, respectively. Under appropriate conditions, the system lasts over 240 h and stays active under 1% concentration of CO 2 . Mechanistic studies reveal that chlorin and chlorinphlorin are two key intermediates in red-light-driven CO 2 reduction, while corresponding porphyrin and bacteriochlorin are much less active forms of chromophores. Using low-energy photons in light-driven reactions is an effective strategy for improving the efficiency of solar energy conversion but molecular systems that mimic such function are extremely rare in non-noble-metal catalysis. Here the authors report fluorinated chlorins as chromophores for CO 2 reduction, which catalytically produce CO under both 630 nm and 730 nm light irradiation.
ISSN:2041-1723
2041-1723
DOI:10.1038/s41467-024-50084-8