Highly selective electrosynthesis of H2O2 by N, O co-doped graphite nanosheets for efficient electro-Fenton degradation of p-nitrophenol

The activity and selectivity of the cathode towards electrosynthesis of H2O2 are critical for electro-Fenton process. Herein, nickel-foam modified with N, O co-doped graphite nanosheets (NO-GNSs/Ni-F) was developed as a cathode for highly efficient and selective electrosynthesis of H2O2. Expectedly, the accumulation of H2O2 at pH= 3 reached 494.2 mg L-1 h-1, with the selectivity toward H2O2 generation reaching 93.0%. The synergistic effect of different oxygen-containing functional groups and N species on the performance and selectivity of H2O2 electrosynthesis was investigated by density functional theory calculations, and the combination of epoxy and graphitic N (EP + N) was identified as the most favorable configuration with the lowest theoretical overpotential for H2O2 generation. Moreover, NO-GNSs/Ni-F was applied in the electro-Fenton process for p-nitrophenol degradation, resulting in 100% removal within 15 min with the kinetic rate constant of 0.446 min-1 and 97.6% mineralization within 6 h. The efficient removal was mainly attributed to the generation of bulk ·OH. Furthermore, NO-GNSs/Ni-F exhibited excellent stability. This work provides a workable option for the enhancement of H2O2 accumulation and the efficient degradation of pollutants in electro-Fenton system.