Selenol-containing two-dimensional perovskite promotes visible-light-driven selective reduction of unsaturated ketones.

Semiconductors have shown growing promise for photocatalytic reactions due to their tunable band structures and efficient charge separation capabilities. Among them, metal halide perovskites (MHPs) have emerged as particularly attractive candidates owing to their intense light absorption and favorable charge transport properties; yet inefficient charge utilization often occurs in MHP-based photocatalysis due to undesired interfacial charge losses and lattice mismatches within the heterostructures. Herein, we report a two-dimensional perovskite (TMHP) photocatalyst, where selenol-functionalized organic cations are integrated into the lattice as both structural components and catalytic sites. This design enables efficient photoinduced charge separation and transfer from the [PbI4]2- layers to the selenol groups, achieving visible-light-driven reduction of α,β-unsaturated ketones with up to 87% yield across diverse substrates. Mechanistic studies reveal a radical-mediated pathway facilitated by the polarized lattice environment. This work demonstrates a new strategy for engineering molecular functionality into semiconductor lattices and creating integrated, efficient photocatalytic systems.