Fluorinated chlorin chromophores for red-light-driven CO 2 reduction.

Autor: Yang S; MOE Key Laboratory of Bioinorganic and Synthetic Chemistry, School of Chemistry, IGCME, Sun Yat-sen University, Guangzhou, China., Yuan H; MOE Key Laboratory of Bioinorganic and Synthetic Chemistry, School of Chemistry, IGCME, Sun Yat-sen University, Guangzhou, China., Guo K; MOE Key Laboratory of Bioinorganic and Synthetic Chemistry, School of Chemistry, IGCME, Sun Yat-sen University, Guangzhou, China., Wei Z; MOE Key Laboratory of Bioinorganic and Synthetic Chemistry, School of Chemistry, IGCME, Sun Yat-sen University, Guangzhou, China., Ming M; MOE Key Laboratory of Bioinorganic and Synthetic Chemistry, School of Chemistry, IGCME, Sun Yat-sen University, Guangzhou, China.; School of Materials Science and Engineering, Xihua University, Chengdu, China., Yi J; MOE Key Laboratory of Bioinorganic and Synthetic Chemistry, School of Chemistry, IGCME, Sun Yat-sen University, Guangzhou, China., Jiang L; MOE Key Laboratory of Bioinorganic and Synthetic Chemistry, School of Chemistry, IGCME, Sun Yat-sen University, Guangzhou, China., Han Z; MOE Key Laboratory of Bioinorganic and Synthetic Chemistry, School of Chemistry, IGCME, Sun Yat-sen University, Guangzhou, China. hanzhiji@mail.sysu.edu.cn.
Jazyk: angličtina
Zdroj: Nature communications [Nat Commun] 2024 Jul 08; Vol. 15 (1), pp. 5704. Date of Electronic Publication: 2024 Jul 08.
DOI: 10.1038/s41467-024-50084-8
Abstrakt: 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.
(© 2024. The Author(s).)
Databáze: MEDLINE
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