Efficient H2O2 electrogeneration from 2-electron oxygen reduction reaction (ORR) represents an important challenge for environmental remediation application. H2O2 production is determined by 2-electron ORR as well as H2O2 decomposition. In this work, a novel strategy based on the systematical investigation on H2O2 decomposition pathways was reported, presenting a drastically improved bulk H2O2 concentration. Results showed that bulk phase disproportion, cathodic reduction, and anodic oxidation all contributed to H2O2 depletion. To decrease the extent of H2O2 cathodic reduction, the pulsed current was applied and proved to be highly effective to lower the extent of H2O2 electroreduction. A systematic study of various pulsed current parameters showed that H2O2 concentration was significantly enhanced by 61.6% under pulsed current of "2s ON + 2s OFF" than constant current. A mechanism was proposed that under pulsed current, less H2O2 molecules were electroreduced when they diffused from the porous cathode to the bulk electrolyte. Further results demonstrated that a proper pulse frequency was necessary to achieve a higher H2O2 production. Finally, this strategy was applied to Electro-Fenton (EF) process with ibuprofen as model pollutant. 75.0% and 34.1% ibuprofen were removed under pulsed and constant current at 10 min, respectively. The result was in consistent with the higher H2O2 and ·OH production in EF under pulsed current. This work poses a potential approach to drastically enhance H2O2 production for improved EF performance on organic pollutants degradation without making any changes to the system except for power mode.
Keywords: Electro-Fenton; Hydrogen peroxide; Ibuprofen; Oxygen reduction reaction; Pulsed current.