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

s Hydrogen peroxide (H 2 O 2 ) electrosynthesis from 2-electron O 2 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 H 2 O 2 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 H 2 O 2 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 O 2 bubbles, which built a gas-liquid-solid interface inside GF and thus enhance the H 2 O 2 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.