Improving photosensitization for photochemical CO2-to-CO conversion

Natl Sci Rev. 2020 May 28;7(9):1459-1467. doi: 10.1093/nsr/nwaa112. eCollection 2020 Sep.

Abstract

Inspired by nature, improving photosensitization represents a vital direction for the development of artificial photosynthesis. The sensitization ability of photosensitizers (PSs) reflects in their electron-transfer ability, which highly depends on their excited-state lifetime and redox potential. Herein, for the first time, we put forward a facile strategy to improve sensitizing ability via finely tuning the excited state of Ru(II)-PSs (Ru-1-Ru-4) for efficient CO2 reduction. Remarkably, [Ru(Phen)2(3-pyrenylPhen)]2+ (Ru-3) exhibits the best sensitizing ability among Ru-1-Ru-4, over 17 times higher than that of typical Ru(Phen)3 2+. It can efficiently sensitize a dinuclear cobalt catalyst for CO2-to-CO conversion with a maximum turnover number of 66 480. Systematic investigations demonstrate that its long-lived excited state and suitable redox driving force greatly contributed to this superior sensitizing ability. This work provides a new insight into dramatically boosting photocatalytic CO2 reduction via improving photosensitization.

Keywords: CO2 reduction; Ru(II) complexes; excited state; photocatalysis; photosensitization.