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<p>Direct photosynthesis of hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>) from air and water using metal/covalent-organic frameworks offers a sustainable alternative to the conventional energy-intensive anthraquinone process. However, current systems suffer from short operational lifetimes typically 10–100 h due to mismatches between O<sub>2</sub> capture efficiency and multielectron redox kinetics. Here, we report a supramolecular platform that integrates O<sub>2</sub> capture, H<sub>2</sub>O<sub>2</sub> synthesis, and in situ utilization, enabling continuous H<sub>2</sub>O<sub>2</sub> production for over 1000 h without sacrificial agents. Mesoporous bromine-substituted COFs are hydrogen-bonded to photothermal MXene, providing organized O<sub>2</sub> docking sites and columnar charge transport via σ-σ interactions and π-π stacking. Through a dual-pathway mechanism, the architecture achieves a competitive H<sub>2</sub>O<sub>2</sub> production rate of 2878 μmol g<sup>−1</sup> h<sup>−1</sup>, alongside complete pollutant removal and durable operation across diverse water sources and outdoor conditions. This work demonstrates a supramolecular design featuring programmable O<sub>2</sub> docking, directional charge transport, and localized H<sub>2</sub>O<sub>2</sub> utilization toward decentralized chemical manufacturing.</p>

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Sustained hydrogen peroxide production via MXene-functionalized supramolecular docking

  • 期刊论文

  • 出版模式：

    开放获取

  • 发表日期：

    2026年3月15日

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  • Jiaxun Sun,
  • Yuanming Zhang,
  • Wanheng Lu,
  • Wei Li Ong,
  • Xinglong Pan,
  • Wentao Song,
  • Zhonghua Li,
  • Zhaosheng Li,
  • Ghim Wei Ho

摘要

Direct photosynthesis of hydrogen peroxide (H2O2) from air and water using metal/covalent-organic frameworks offers a sustainable alternative to the conventional energy-intensive anthraquinone process. However, current systems suffer from short operational lifetimes typically 10–100 h due to mismatches between O2 capture efficiency and multielectron redox kinetics. Here, we report a supramolecular platform that integrates O2 capture, H2O2 synthesis, and in situ utilization, enabling continuous H2O2 production for over 1000 h without sacrificial agents. Mesoporous bromine-substituted COFs are hydrogen-bonded to photothermal MXene, providing organized O2 docking sites and columnar charge transport via σ-σ interactions and π-π stacking. Through a dual-pathway mechanism, the architecture achieves a competitive H2O2 production rate of 2878 μmol g−1 h−1, alongside complete pollutant removal and durable operation across diverse water sources and outdoor conditions. This work demonstrates a supramolecular design featuring programmable O2 docking, directional charge transport, and localized H2O2 utilization toward decentralized chemical manufacturing.