Department of Environmental Engineering, Faculty of Environment and Life, 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, Faculty of Environment and Life, 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.
Chemosphere. 2023 Aug;332:138860. doi: 10.1016/j.chemosphere.2023.138860. Epub 2023 May 5.
In sulfate radical-based advanced oxidation processes (SR-AOPs), high-efficiency and perdurable materials have drawn considerable interest for use as cathodes, which can effectively degrade refractory organic contaminants through the synergistic electro-activation and transition metal activation of persulfate (PS). Here, the FeCuO@C modified composite cathode (FeCuO@C/AGF) was synthesized via the solvothermal and thermal treatment method based on the CuFe-MOF-74 structure, and the electro-activation PS process (EC/FeCuO@C/AGF/PS) was developed to effectively remove atrazine (ATZ). The surface morphology, electrochemical characteristics, chemical composition, crystal structure, and electrode surface wettability of FeCuO@C/AGF were investigated. It was found that the proposed EC/FeCuO@C/AGF/PS process can successfully remove 100% of ATZ in 20 min at a low current density (2 mA cm) and a low PS concentration (0.4 mM), and PS is successfully activated by combining the electrical and transition metal synergistic activation. The FeCuO@C/AGF cathode exhibits outstanding catalytic functionality over a broad pH range (2-9) and remains stable over five successive cycles. Additionally, the active species involved in the reaction as well as the potential ATZ degradation reaction mechanisms and pathways are discussed. Electrochemical oxidation is a process in which both radicals (SO, ·OH, and O) and non-radical (O) participate in the degradation of ATZ. The intermediates of the ATZ degradation process were studied upon the toxicity changing, and the toxicity of the intermediates was found to be reduced during degradation. These results present a novel approach toward the establishment of an effective and reliable electrode in SR-AOPs that can efficiently treat pesticide wastewater.
在硫酸根自由基基高级氧化工艺 (SR-AOPs) 中，高效且持久的材料作为阴极引起了相当大的兴趣，通过协同电激活和过硫酸盐 (PS) 的过渡金属激活，可以有效地降解难处理的有机污染物。在这里，基于 CuFe-MOF-74 结构，通过溶剂热和热处理方法合成了 FeCuO@C 修饰的复合阴极 (FeCuO@C/AGF)，并开发了电激活 PS 过程 (EC/FeCuO@C/AGF/PS) 以有效去除莠去津 (ATZ)。研究了 FeCuO@C/AGF 的表面形貌、电化学特性、化学成分、晶体结构和电极表面润湿性。结果发现，在低电流密度 (2 mA cm) 和低 PS 浓度 (0.4 mM) 下，该提议的 EC/FeCuO@C/AGF/PS 过程可以在 20 分钟内成功去除 100%的 ATZ，并且 PS 通过电和过渡金属协同激活成功被激活。FeCuO@C/AGF 阴极在较宽的 pH 范围 (2-9) 内表现出出色的催化功能，并且在五个连续循环中保持稳定。此外，还讨论了反应中涉及的活性物质以及潜在的 ATZ 降解反应机制和途径。电化学氧化是一种自由基 (SO、·OH 和 O) 和非自由基 (O) 都参与 ATZ 降解的过程。研究了 ATZ 降解过程中的中间产物以及毒性变化，发现中间产物在降解过程中的毒性降低。这些结果为在 SR-AOPs 中建立有效且可靠的电极提供了一种新方法，可以有效地处理农药废水。
