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. Programmable supramolecular COF/MXene assemblies integrate convenient H2O2 photoproduction with photothermal units, realizing long-term O2 capture, in situ H2O2 synthesis and utilization toward decentralized green chemical manufacturing.