Precise Design of Covalent Organic Frameworks for Electrocatalytic Hydrogen Peroxide Production

Electrochemical synthesis of H₂ O₂ with high productivity is a significant challenge in electrocatalysis. Herein, we develop Mg-ion contained covalent organic frameworks (MgP-DHTA-COF), comprising stacked 2D layers, well-defined skeletons, and well-ordered monodispersed active sites, for the electrocatalytic production of H₂ O₂ directly from O₂ and H₂ O. The precise-designed MgP-DHTA-COF achieves H₂ O₂ selectivity up to 96%, high Faradaic efficiency of 91% and reliable stability for H₂ O₂ synthesis in 0.10 mol L^-1 KOH aqueous solution. Both experiments and simulations demonstrate that the pyrrolic-N fixed Mg ions in the knots promote the reactivity of COF and enhance the adsorption ability of OOH*. This work provides a valuable example for the design of an efficient electrocatalyst based on COFs for H₂ O₂ production.