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.