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

Yilin Jiang, Ruonan Xi, Jinlin Yin, Chen Sun, Yukong Li, Chao Wu, Chi Zhang () and Honghan Fei ()
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Yilin Jiang: Tongji University
Ruonan Xi: Tongji University
Jinlin Yin: Tongji University
Chen Sun: Tongji University
Yukong Li: Tongji University
Chao Wu: Tongji University
Chi Zhang: Tongji University
Honghan Fei: Tongji University

Nature Communications, 2025, vol. 16, issue 1, 1-13

Abstract: 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.

Date: 2025
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DOI: 10.1038/s41467-025-60954-4

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