A layered lead halide framework intercalated with Ru(bpy)3 for efficient CO2 photoreduction
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 pre...
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| Format: | Article |
| Language: | English |
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Nature Portfolio
2025-07-01
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| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-025-60954-4 |
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| _version_ | 1849402205658939392 |
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| author | Yilin Jiang Ruonan Xi Jinlin Yin Chen Sun Yukong Li Chao Wu Chi Zhang Honghan Fei |
| author_facet | Yilin Jiang Ruonan Xi Jinlin Yin Chen Sun Yukong Li Chao Wu Chi Zhang Honghan Fei |
| author_sort | Yilin Jiang |
| collection | DOAJ |
| description | 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. |
| format | Article |
| id | doaj-art-0bde29600cc046bb9327bf4e627ec99c |
| institution | Kabale University |
| issn | 2041-1723 |
| language | English |
| publishDate | 2025-07-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Nature Communications |
| spelling | doaj-art-0bde29600cc046bb9327bf4e627ec99c2025-08-20T03:37:37ZengNature PortfolioNature Communications2041-17232025-07-0116111310.1038/s41467-025-60954-4A layered lead halide framework intercalated with Ru(bpy)3 for efficient CO2 photoreductionYilin Jiang0Ruonan Xi1Jinlin Yin2Chen Sun3Yukong Li4Chao Wu5Chi Zhang6Honghan Fei7School of Chemical Science and Engineering, Shanghai Key Laboratory of Chemical Assessment and Sustainability, Tongji UniversitySchool of Chemical Science and Engineering, Shanghai Key Laboratory of Chemical Assessment and Sustainability, Tongji UniversitySchool of Chemical Science and Engineering, Shanghai Key Laboratory of Chemical Assessment and Sustainability, Tongji UniversitySchool of Chemical Science and Engineering, Shanghai Key Laboratory of Chemical Assessment and Sustainability, Tongji UniversitySchool of Chemical Science and Engineering, Shanghai Key Laboratory of Chemical Assessment and Sustainability, Tongji UniversitySchool of Chemical Science and Engineering, Shanghai Key Laboratory of Chemical Assessment and Sustainability, Tongji UniversitySchool of Chemical Science and Engineering, Shanghai Key Laboratory of Chemical Assessment and Sustainability, Tongji UniversitySchool of Chemical Science and Engineering, Shanghai Key Laboratory of Chemical Assessment and Sustainability, Tongji UniversityAbstract 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.https://doi.org/10.1038/s41467-025-60954-4 |
| spellingShingle | Yilin Jiang Ruonan Xi Jinlin Yin Chen Sun Yukong Li Chao Wu Chi Zhang Honghan Fei A layered lead halide framework intercalated with Ru(bpy)3 for efficient CO2 photoreduction Nature Communications |
| title | A layered lead halide framework intercalated with Ru(bpy)3 for efficient CO2 photoreduction |
| title_full | A layered lead halide framework intercalated with Ru(bpy)3 for efficient CO2 photoreduction |
| title_fullStr | A layered lead halide framework intercalated with Ru(bpy)3 for efficient CO2 photoreduction |
| title_full_unstemmed | A layered lead halide framework intercalated with Ru(bpy)3 for efficient CO2 photoreduction |
| title_short | A layered lead halide framework intercalated with Ru(bpy)3 for efficient CO2 photoreduction |
| title_sort | layered lead halide framework intercalated with ru bpy 3 for efficient co2 photoreduction |
| url | https://doi.org/10.1038/s41467-025-60954-4 |
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