Efficient Electrochemical Hydrogen Peroxide Production\nfrom Molecular Oxygen on Nitrogen-Doped Mesoporous Carbon Catalysts

Abstract

Electrochemical hydrogen\nperoxide (H₂O₂)\nproduction by two-electron oxygen reduction is a promising alternative\nprocess to the established industrial anthraquinone process. Current\nchallenges relate to finding cost-effective electrocatalysts with\nhigh electrocatalytic activity, stability, and product selectivity.\nHere, we explore the electrocatalytic activity and selectivity toward\nH₂O₂ production of a number of distinct nitrogen-doped\nmesoporous carbon catalysts and report a previously unachieved H₂O₂ selectivity of ∼95–98% in acidic\nsolution. To explain our observations, we correlate their structural,\ncompositional, and other physicochemical properties with their electrocatalytic\nperformance and uncover a close correlation between the H₂O₂ product yield and the surface area and interfacial\nzeta potential. Nitrogen doping was found to sharply boost H₂O₂ activity and selectivity. Chronoamperometric H₂O₂ electrolysis confirms the exceptionally high\nH₂O₂ production rate and large H₂O₂ faradaic selectivity for the optimal nitrogen-doped\nCMK-3 sample in acidic, neutral, and alkaline solutions. In alkaline\nsolution, the catalytic H₂O₂ yield increases\nfurther, where the production rate of the HO₂^– anion reaches a value as high as 561.7 mmol g_catalyst^–1 h^–1 with H₂O₂ faradaic selectivity above 70%.\nOur work provides a guide for the design, synthesis, and mechanistic\ninvestigation of advanced carbon-based electrocatalysts for H₂O₂ production.