Janus graphite felt cathode dramatically enhance the H2O2 yield from O2 electroreduction by the hydrophilicity-hydrophobicity regulation.

Hydrogen peroxide (H2O2) electrosynthesis from 2-electron O2 reduction reaction (2eORR) is widely regarded as a promising alternative to the current industry-dominant anthraquinone process. Design and fabrication of effective, low-cost carbon-based electrodes is one of the priorities. Many previous work well confirmed that hydrophilic carbon-based electrodes are preferable for 2eORR. Here, we proposed a strategy of hydrophilicity-hydrophobicity regulation. By using commercially available graphite felt (GF) as electrodes, we showed that both hydrophilic GF, hydrophobic GF, and Janus GF yielded significantly higher H2O2 production, which is 7.3 times, 7.6 times, and 7.7 times higher than the original GF, respectively. Results showed that currents and stirring rates affect the H2O2 yields. The enhancement of hydrophilic GF is due to the incorporation of oxygen-containing functional groups, while the hydrophobic and Janus GF comes from the locally confined O2 bubbles, which built a gas-liquid-solid interface inside GF and thus enhance the H2O2 formation kinetics. Finally, the effectiveness of the hydrophilicity-hydrophobicity regulation concept was tested in Electro-Fenton process by removing typical dyes and antibiotics. This work supply an effective but facile strategy to enhance the performance of carbon-based electrodes towards 2eORR by regulating the micro-environment of electrodes.