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<p>Lead halide perovskites are promising for artificial photosynthesis but suffer from aqueous instability. Here, we stabilize CsPbI<sub>3</sub> quantum dots within a hydrophobic chlorine-functionalized covalent organic framework through multisite atomic-chlorine passivation, forms dual Cl-Pb coordination and Cl-I halogen bonding at the interface. This suppresses ionic migration while creating a gas-solid-liquid triphase interface for enhanced O<sub>2</sub> diffusion. The resulting S-scheme heterojunction spatially separates carriers to concurrently drive two-electron oxygen reduction and water oxidation for H<sub>2</sub>O<sub>2</sub> synthesis without sacrificial agents. The system achieves production rates of 20.37 mmol h<sup>−1</sup> g<sup>−1</sup> in seawater, with a solar-to-chemical conversion efficiency of 1.38%, and operates stably for 20 h. Importantly, natural sunlight tests yield 11.7 mmol L<sup>−1</sup> H<sub>2</sub>O<sub>2</sub> in 10 h. Mechanistic studies confirm synergistic interfacial charge transfer and dual-reaction pathways via both oxygen reduction and water oxidation. This work demonstrates an approach for robust perovskite-based photocatalysts toward solar-driven chemical synthesis from seawater.</p>

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Multisite atomic-chlorine-passivation stabilizes perovskite interfaces for efficient H2O2 photosynthesis from seawater

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年3月15日

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  • Genping Meng,
  • Shuai Wei,
  • Ning Li,
  • Yuhui Yin,
  • Bin Dong,
  • Shihao Sun,
  • Guowen Hu,
  • Hao Wang,
  • Baodui Wang

摘要

Lead halide perovskites are promising for artificial photosynthesis but suffer from aqueous instability. Here, we stabilize CsPbI3 quantum dots within a hydrophobic chlorine-functionalized covalent organic framework through multisite atomic-chlorine passivation, forms dual Cl-Pb coordination and Cl-I halogen bonding at the interface. This suppresses ionic migration while creating a gas-solid-liquid triphase interface for enhanced O2 diffusion. The resulting S-scheme heterojunction spatially separates carriers to concurrently drive two-electron oxygen reduction and water oxidation for H2O2 synthesis without sacrificial agents. The system achieves production rates of 20.37 mmol h−1 g−1 in seawater, with a solar-to-chemical conversion efficiency of 1.38%, and operates stably for 20 h. Importantly, natural sunlight tests yield 11.7 mmol L−1 H2O2 in 10 h. Mechanistic studies confirm synergistic interfacial charge transfer and dual-reaction pathways via both oxygen reduction and water oxidation. This work demonstrates an approach for robust perovskite-based photocatalysts toward solar-driven chemical synthesis from seawater.