Electrosynthesis of >20 g/L H₂O₂ from Air

Hydrogen peroxide (HP) production via electrochemical oxygen reduction reaction (ORR-HP) is a critical reaction for energy storage and environmental remediation. The onsite production of high-concentration H₂O₂ using gas diffusion electrodes (GDEs) fed by air is especially attractive. However, many studies indicate that the air-GDE combination could not produce concentrated H₂O₂, as the [H₂O₂] leveled off or even decreased with the increasing reaction time. This study proves that the limiting factors are not the oxygen concentration in the air but the anodic and cathodic depletion of the as-formed H₂O₂. We proved that the anodic depletion could be excluded by adopting a divided electrolytic cell. Furthermore, we demonstrated that applying poly(tetrafluoroethylene) (PTFE) as an overcoating rather than a catalyst binder could effectively mitigate the cathodic decomposition pathways. Beyond that, we further developed a composite electrospun PTFE (E-PTFE)/carbon black (CB)/GDE electrode featuring the electrospun PTFE (E-PTFE) nanofibrous overcoating. The E-PTFE coating provides abundant triphase active sites and excludes the cathodic depletion reaction, enabling the production of >20 g/L H₂O₂ at a current efficiency of 86.6%. Finally, we demonstrated the efficacy of the ORR-HP device in lake water remediation. Cyanobacteria and microcystin-LR were readily removed along with the onsite production of H₂O₂.