Chiral Chlorophyll-Inspired Clusters Steering Electron Transfer for Enhanced CO2 Photoreduction

Abstract

Recombination of free charges in metal-oxygen cluster complexes reduces the number of available photoinduced carriers, thus limiting photovoltaic efficiency. Inspired by the structure of natural chlorophyll, applying the self-assembly molecular puzzle strategy to photocatalyst design is a promising approach to uncover the secrets of high catalytic activity. Specifically, 2,6-diacetyl pyridine bis(semicarbazone) (DAPSC) and Co coordination serve as the "head" of the artificial chlorophyll molecule, 1,3-bis(4-pyridyl)propane (bpp) molecules act as the "tail," synthesizing two new artificial biomimetic chlorophyll molecular photocatalysts, D- and L-Co-BPP. The induced spin polarization of the chiral structure promotes carrier lifetime extension and inhibits electron-hole recombination, thereby enhancing photocatalytic performance. Fortunately, the photocatalytic activity of biomimetic photocatalysts Co-BPP on pure CO2 is significant (65061.6 μmol g-1) and exhibits decent activity at 10% concentrations. This study explores new avenues for utilizing artificial bionic photocatalysts to convert CO2.