Abstract

Bifunctional cathodes have attracted widespread interest in the heterogeneous electro-Fenton (hetero-EF) process. In this study, the bifunctional composite cathode co-modified with N-doped carbon CoFe alloy (CoFe@NC) and carbon nanotubes (CNTs), designated as CoFe@NC-CNTs/CNTs/NF, integrating hydrogen peroxide (H2O2) synthesis and catalysis, was prepared for efficient degradation of atrazine (ATZ) under the near-neutral condition (pHi = 5.9). The morphology properties, crystal structure, microstructures, and elemental composition were determined. The influences of current density, initial pH value, different anions, and water matrix on the removal of ATZ were systematically studied. In the hetero-EF process, high removal efficiencies of ATZ can be achieved over the broad pH range (3–9) under the current density of 4.5 mA cm−2. The removal efficiency of ATZ remained at 90.2 ± 0.3% after 8 cycles under the near-neutral condition (pHi = 5.9). Radical quenching tests and EPR spectra have verified that both free radical pathways such as superoxide anion (O2·-) and hydroxyl radical (·OH) and non-radical pathway such as singlet oxygen (1O2) contributed to ATZ removal. The degradation pathways and catalytic mechanism were proposed. Toxicity evaluation and Escherichia coli growth test showed that the toxicity gradually decreased during the degradation process. This work provided a new thought for developing an efficient and stable bifunctional cathode to construct an in-situ hetero-EF system for pollutants removal over the wide pH range.

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