Li Xianpeng, Yang Jingjie, Shi Xuelin, Sun Zhirong
Department of Environmental Engineering, Beijing University of Technology, Beijing, 100124, PR China; National Engineering Laboratory for Advanced Municipal Wastewater Treatment and Reuse Technology, Beijing University of Technology, Beijing, 100124, PR China.
Department of Environmental Engineering, Beijing University of Technology, Beijing, 100124, PR China; National Engineering Laboratory for Advanced Municipal Wastewater Treatment and Reuse Technology, Beijing University of Technology, Beijing, 100124, PR China.
Environ Res. 2025 Feb 1;266:120577. doi: 10.1016/j.envres.2024.120577. Epub 2024 Dec 7.
To enhance the contaminant removal efficiency of the electro-Fenton (E-Fenton) process, a nitrogen and phosphorus co-doped graphite felt (NPGF) cathode was synthesized using an anodic oxidation technique. An ascorbic acid-coupled NPGF E-Fenton system was then established for the degradation of ciprofloxacin (CIP). The NPGF cathode featured abundant oxygen-containing functional groups (such as -COOH and -OH), which enhanced the selectivity of oxygen reduction and facilitated the formation of HO. The introduction of N and P doping disrupted the charge balance within the carbon framework, accelerating electron transfer. Together, the NPGF electrode and ascorbic acid enhanced the cycling of Fe/Fe while preventing the formation of iron sludge. Under optimal conditions (ascorbic acid concentration of 0.3 mM, current density of 2.0 mA cm, pH of 3.0, aeration rate of 0.6 L min, and Fe concentration of 0.2 mM), CIP was completely removed within 20 min. The NPGF electrode exhibited excellent stability, maintaining 95.35% CIP removal even after 8 cycles. Analysis revealed that singlet oxygen primarily mediated the degradation of CIP, with its concentration measured at 1.23 × 10 M. Density functional theory was used to analyze the characteristics and potential attack sites of CIP, enabling the proposal of plausible degradation pathways. Toxicity simulations and Escherichia coli growth inhibition experiments demonstrated a reduction in the toxicity of CIP and its intermediate products. This study offers a valuable reference for improving the efficiency of E-Fenton technology in antibiotic wastewater treatment.
为提高电芬顿(E-Fenton)工艺的污染物去除效率,采用阳极氧化技术合成了氮磷共掺杂石墨毡(NPGF)阴极。然后建立了抗坏血酸耦合的NPGF E-Fenton体系用于降解环丙沙星(CIP)。NPGF阴极具有丰富的含氧官能团(如-COOH和-OH),提高了氧还原的选择性并促进了羟基自由基(HO)的形成。氮和磷掺杂的引入打破了碳骨架内的电荷平衡,加速了电子转移。NPGF电极和抗坏血酸共同作用增强了Fe/Fe的循环,同时防止了铁泥的形成。在最佳条件下(抗坏血酸浓度为0.3 mM、电流密度为2.0 mA cm、pH为3.0、曝气速率为0.6 L min、Fe浓度为0.2 mM),20分钟内CIP被完全去除。NPGF电极表现出优异的稳定性,即使在8个循环后仍保持95.35%的CIP去除率。分析表明,单线态氧主要介导了CIP的降解,其浓度为1.23×10 M。采用密度泛函理论分析了CIP的特性和潜在攻击位点,从而提出了合理的降解途径。毒性模拟和大肠杆菌生长抑制实验表明CIP及其中间产物的毒性降低。本研究为提高E-Fenton技术处理抗生素废水的效率提供了有价值的参考。