Towards electron-transfer-driven peracetic acid oxidation: Catalytic performance adaptation of reduced graphene oxide to explosive thermal exfoliation

Direct electron transfer (DET)-mediated carbon/peracetic acid (PAA) oxidation systems are gaining momentum in water treatment owing to high selectivity and robustness in complex water matrices. However, the development of reaction-oriented and high-performance carbon catalysts for PAA oxidation is hindered by a limited understanding of the fundamental relationship between carbon structure and PAA activation performance. In this work, we focused on exploring the influence cascade of thermal annealing, especially explosive thermal exfoliation, on the catalytic performance adaptation of reduced graphene oxide (rGO) in PAA oxidation. By performing structure-performance relationship studies and Pearson correlation analyses, the improved catalytic efficacy of rGO is attributed to the induced high specific surface area (SSA) and pore volume of rGO in explosive thermal exfoliation. Large SSA and pore volume of rGO reinforce the DET pathway via the elevated PAA adsorption quantity and subsequent enhanced oxidative potential of the rGO-PAA complex, which are critical premises in initiating DET. Furthermore, increased annealing temperatures can tailor the graphitization level and functional group content of rGO, leading to the improved electrical conductivity of rGO, another crucial factor in DET-mediated rGO/PAA oxidation. This study emphasizes the key role of carbon physicochemical properties in PAA activation, providing insights into the rational design of DET-oriented carbon/PAA oxidation systems for fast water decontamination.