Abstract
• Cu/CuFe 2 O 4 with different Cu 0 ratios were synthesized by a solvothermal method. • Cu/CuFe 2 O 4 integrated GF was developed for cathode of the heterogeneous EF process. • PTFE improved the oxygen utilization rate and stability of the composite cathode. • Cu 0 as electron-rich centers can accelerate redox cycling of Fe(III)/Fe(II). The development of transition metal oxide-based integrated carbonaceous materials for use as bifunctional electrodes of high stability and activity in the heterogeneous electro-Fenton (EF) process is supposed to have great potential in environmental governance. Herein, Cu/CuFe 2 O 4 (CCFO) with different Cu 0 ratios were synthesized by a facile one-step solvothermal approach. These materials were subsequently used to fabricate modified graphite felt through the polytetrafluoroethylene (PTFE)-bonding technique. Importantly, with its hydrophobicity PTFE effectively inhibited metal leaching from the thus obtained cathodes and improved the oxygen utilization rate. Cathode performance in EF-based tetracycline (TC) degradation was found to increase with Cu 0 ratio. The observed increase in activity was attributed to Cu 0 enhancing the 2-electron oxygen reduction reaction selectivity (i.e., H 2 O 2 production) and endowing the cathode with abundant electron-rich centers that accelerated active Fe(II) regeneration, causing rapid conversion of H 2 O 2 to hydroxyl radical ( OH). The possible TC mineralization pathway was inferred by liquid chromatography–mass spectrometry (LC–MS) analysis, and a catalytic mechanism of the heterogeneous EF process was proposed. The most effective cathode fabricated displayed high stability even at pH 3 (0.84 ± 0.11 mg/L Fe and 1.35 ± 0.17 mg/L Cu leaching) and exhibited nearly 80% TC removal efficiency after five oxidation cycles, demonstrating its potential use in heterogeneous EF technology for efficient and durable wastewater treatment.
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