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Seawater Electrosynthesis of Hydrogen Peroxide at Industrial‐level Current Densities Enabled by Pentagonal Defect‐Rich Nanocarbon with Chlorine Doping

Hongshang Hu, Chang Zhang, Huiyao Qi, Lilong Zhang, Muneerah Alomar, Lipiao Bao, Xing Lu, Jian Zhang

2025Angewandte Chemie International Edition12 citationsDOI

Abstract

Abstract The electrosynthesis of hydrogen peroxide (H 2 O 2 ) via two‐electron oxygen reduction reaction (2e – ORR) in seawater shows great prospects. However, designing an electrocatalyst with high activity and selectivity, resistance to seawater corrosion, and even stable operation at industrial currents (≥300 mA cm −2 ), remains a critical challenge. In this work, we report a pentagonal defect‐rich nanocarbon with chlorine‐doping (Cl‐PDC) by tailoring fullerene (C 60 ) precursors via the molten salt method. The as‐prepared Cl‐PDC catalyst achieves a record H 2 O 2 yield of 74.61 mol g cat −1 h −1 at a current density of 800 mA cm −2 with a nearly 100% Faradaic efficiency, outperforming among all previously reported catalysts in simulated seawater or neutral environments. Remarkably, the Cl‐PDC‐based electrode maintains operational stability over 400 h in simulated seawater, and enables rapid disinfection and pollutant degradation. Theoretical calculations and experimental analysis reveal that the synergy between the intrinsic pentagonal defects and Cl doping modulates the electronic structure of the carbon framework, optimizing *OOH intermediate adsorption, and introduces the localized negative charge to suppress Cl − poisoning at active sites. This work paves the way for sustainable seawater H 2 O 2 production and marine environmental protection.

Topics & Concepts

SeawaterMaterials scienceCatalysisElectrocatalystHydrogen peroxideInorganic chemistryElectrochemistryChemical engineeringChlorineElectrosynthesisDopingElectrolyteCarbon fibersFaraday efficiencyRedoxOxygen evolutionHydrogenYield (engineering)Current densityPolyoxometalateHalideCathodic protectionElectrodeOxygenReversible hydrogen electrodeElectrolysis of waterWater splittingFullereneAdvanced oxidation water treatmentElectrocatalysts for Energy ConversionAdvanced battery technologies research