Sustained hydrogen peroxide production via MXene-functionalized supramolecular docking

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.