Work

A layered lead halide framework intercalated with Ru(bpy)3 for efficient CO2 photoreduction

Year: 2025

Type: article

Abstract: Three-dimensional lead halide hybrids exhibit excellent photophysical properties but suffer from inherent instability. In contrast, two-dimensional layered lead halides offer enhanced environmental stability, yet their strongly bound excitons restrict efficient charge transport. Here we present a covalent intercalation strategy involving the benchmark photosensitizer [Ru(bpy)3]2+ into a layered lead halide framework, featuring cationic [Pb23X42]4+ (X− = Cl− or Br−) layers pillared by [Ru(bpy)3]2+ ligands via Pb2+-carboxylate coordination. This hybrid material achieves nearly full visible-light absorption and efficient photoinduced charge transfer from [Ru(bpy)3]2+ to the lead halide layers. This affords efficient CO2-to-CO photoreduction with an apparent quantum efficiency of ~3.0% at 500 nm, exceeding the performance of all previously reported organolead halide photocatalysts. Mechanistic studies indicate that the [Ru(bpy)3]2+ ligands enhance charge transport to Pb2+ sites, facilitating CO2 activation and reducing the reaction barrier for the *COOH intermediate. This work establishes a paradigm for intercalation chemistry in robust layered lead halide hybrids. A layered hybrid lead halide intercalated with Ru(bpy)32+ is assembled through Pb2+-carboxylate coordination. The material has broad visible light absorption and drives photocatalytic CO2 reduction to CO with a quantum yield of ~3.0% at 500 nm.

Source: Nature Communications

DOI: 10.1038/s41467-025-60954-4