Hydrogen-bonded organic framework@conductive metal-organic framework heterostructures for ampere-level hydrogen...

Electrochemical two-electron oxygen reduction reaction (2e^- ORR) in neutral environments holds remarkable promise for sustainable hydrogen peroxide (H₂O₂) production. However, its practical application is largely hindered due to the scarcity of electrocatalysts with high selectivity and durability under ampere-level current densities. Herein, a hydrogen-bonded organic framework@conductive metal-organic framework (HOF@cMOF) heterostructure is designed for industrial-level H₂O₂ electrosynthesis. Through integrating DAT-HOF (DAT=diaminotriazole) and Co-cMOF, Co-N bonds formed at the heterointerface modulates the electronic structure of Co sites, optimizing the adsorption strength of oxygen intermediates with improved activity and selectivity. Besides, the formation of built-in electric field drives the proton migration from DAT-HOF to Co-cMOF, facilitating the O₂ protonation to H₂O₂ at Co sites. In further combination with the high proton donation capability of DAT-HOF and high conductivity of Co-cMOF, efficient H₂O₂ production is achieved with a H₂O₂ Faradic efficiency of 97.1 ± 0.4%, a H₂O₂ yield of 738.9 mg h⁻¹ cm⁻² and a long-term durability over 100 h at 1200 mA cm⁻². This work offers a high-performance electrocatalyst for promoting the industrial implementation of H₂O₂ electrosynthesis.