Water Oxidation to H2O2 on Surface-Modified Carbon Cloth Electrode

Abstract

The electrochemical water oxidation reaction (WOR) represents a promising route for on-site synthesis of hydrogen peroxide (H₂O₂), but its practical application is hindered by limited activity, selectivity, and insufficient mechanistic understanding. Herein, we report a polyvinylidene fluoride-modified carbon cloth (PVDF/CC) electrocatalyst that achieves a Faradaic efficiency of 91% toward H₂O₂ at 2.75 V vs. RHE, with a high current density of 131 mA cm^-2 and accumulated H₂O₂ concentration of 52 mM. Through a combination of in situ ATR-FTIR spectroscopy and isotope labeling experiments, we confirm the involvement of a carbonate-mediated reaction pathway. Theoretical calculations further reveal that fluorine-induced hydrogen bonds between PVDF and surface hydroxyl groups promote hydroxyl adsorption and facilitate the formation of HCO₄^- intermediates. This work offers a simple and cost-effective strategy for efficient electrochemical H₂O₂ production via the WOR pathway