Selective photocatalyitic CO2 reduction to acetic acid on chiral mesostructured ZnIn2S4

Abstract: Acetic acid, an important industrial chemical, is a key target for CO2 reduction due to its dual role in carbon utilization and chemical feedstock supply.Although acetic acid can be produced by prhotocatalytic CO2 redcution. Among other multicarbon products, it is typically a low-yieleded product due to competing reaction pathways and inefficient C-C coupling. Herein, we report a chiral mesostructured ZnIn2S4 photocatalyst that achieves a remarkable acetic acid yield of 962 umolg-1h-1 with a high selectivity of 97.3%. The yield is ten times higher than the current highest reported value, while attaining state-of-the-art selectivity. The remarkable The remarkable productivity arises from synergistic cooperation between chiral structure and sulfur (S) sites of CMZI. Chirality-induced spin polarization in CMZI stabilizes the key triplet OCCO intermediate, significantly promoting C-C coupling efficiency. Theoretical calculations reveal that the S sites on (102) crystal facets of ZnIn2S4 exhibit thermodynamic and kinetic preferences for acetic acid formation. This work offers critical insights into catalytic strategies for CO2 reduction that could enable the synthesis and scalable production of various multicarbon products.