High-efficiency metal-free electro-Fenton system on oxygenated graphene-based floating electrodes

Metal-free electro-Fenton (EF) are a promising technology for environmental remediation. This paper reports a novel EF modified with oxygenated graphene aerogel used as a floating electrode for efficient degradation of bisphenol A (BPA) through improved H2O2 yield combined with activation of hydroxyl radical (·OH) production. Impressively, the floating configuration of the electrodes allowed oxygen from the air to diffuse naturally into the reaction interface, reducing additional aeration energy consumption. The current efficiency of the floating system for H2O2 production was 40 times higher than the conventional vertical mode. The pollutant degradation trend exhibited a positive correlation with the ·OH production performance of the electrode. The modified catalyst system achieved the highest ·OH yield of 76.48 μM within 60 min, which was 2.72 times greater than that of the catalyst-free (28.10 μM) and 2.06 times higher than that of the unmodified catalyst (37.19 μM). Experiments and theoretical calculations indicated that the oxygen-containing functional groups introduced the graphene skeleton created new sites for in situ activation of electrogenerated H2O2, resulting in increased ·OH production. The primary activation sites were identified as the = O and –COOH groups, with the = O edges playing a particularly significant role. This system offers long-lasting stability and avoids secondary pollution, making it ideal for green environmental remediation compared to the traditional EF process.