Yang Shuang,Yuan Huiqing,Guo Kai,Wei Zuting,Ming Mei,Yi Jinzhi,Jiang Long,Han Zhiji
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.
Photoresponsive amphiphiles are functionalised with photoactivating units, enabling dynamic controls of hierarchical supramolecular systems with a non-invasive photo-stimulation. Limited visible-light driven photoresponsive amphiphiles were developed, while biomedical applications of well-developed UV-light driven photoresponsive amphiphiles are hindered due to bio-damaging effect. Herein, we report newly designed red-light responsive N, N′ -alkyl-aryl-substituted indigo amphiphiles (IA), showing excellent photoswitchability and photostability in organic media. Upon dissolution of IA in aqueous media, supramolecular nanostructures are constructed at pH 7. Though photoresponsiveness of IA is slightly compromised, co-solvent and co-assembly of IA enable supramolecular transformations from vesicle to irregular aggregate in aqueous media. Through investigation of the photoisomerisation and supramolecular transformation processes, this work could provide as a new strategy towards the development of red-light controlled biomedical soft functional materials .
危险品化学品经营许可证（带存储）