State Key Laboratory of Metastable Materials Science and Technology, Hebei Key Laboratory of Heavy Metal Deep-Remediation in Water and Resource Reuse, School of Environmental and Chemical Engineering, Yanshan University, Qinhuangdao, 066004, PR China.
State Key Laboratory of Metastable Materials Science and Technology, Hebei Key Laboratory of Heavy Metal Deep-Remediation in Water and Resource Reuse, School of Environmental and Chemical Engineering, Yanshan University, Qinhuangdao, 066004, PR China.
Chemosphere. 2023 Apr;319:138025. doi: 10.1016/j.chemosphere.2023.138025. Epub 2023 Jan 31.
We applied gallic acid (GA) as the complexing agent to stabilizing the regeneration of Fe during the Fe/peroxydisulfate (PDS) Fenton-like reaction for promoting the removal of metronidazole (MTZ). This research evaluated the elimination of MTZ by optimizing the dose of GA and Fe and pH condition. MTZ removal reached 83% at the GA: Fe molar ratio of 1:1 (30 μM) and initial pH 5 and 6.2 after 120 min, and the kinetics showed two degradation phases (k = 0.09636 for the rapid stage and k = 0.01056 for the slow stage). The Fe and GA complexes could expand the range of pH applicability and effectively stabilize the regeneration of Fe, which ultimately promoted the decontamination of MTZ. Sulfate radical (SO), hydroxyl radicals, and singlet oxygen were proved to exist in this ternary system and contribute to MTZ removal, and SO played the dominant role. Furthermore, the possible pathways and mechanisms for MTZ degradation were proposed, and the simulation result indicated that the toxicity of degradation intermediates of MTZ were declined. The GA assisted Fe/PDS system provided an improved promising advanced oxidation process for organic wastewater disposal.
我们应用没食子酸(GA)作为络合剂来稳定铁在铁/过二硫酸盐(PDS)类 Fenton 反应中的再生,以促进甲硝唑(MTZ)的去除。本研究通过优化 GA 和 Fe 的剂量以及 pH 值条件来评估 MTZ 的去除效果。在 GA:Fe 摩尔比为 1:1(30 μM)和初始 pH 值为 5 和 6.2 的条件下,经过 120 min 后,MTZ 的去除率达到 83%,动力学显示有两个降解阶段(快速阶段的 k 值为 0.09636,慢速阶段的 k 值为 0.01056)。Fe 和 GA 配合物可以扩大 pH 值适用范围,并有效地稳定 Fe 的再生,从而最终促进 MTZ 的去除。证明在这个三元体系中存在硫酸根自由基(SO)、羟基自由基和单线态氧,并有助于 MTZ 的去除,其中 SO 起主要作用。此外,还提出了 MTZ 降解的可能途径和机制,模拟结果表明 MTZ 降解中间产物的毒性降低。GA 辅助的 Fe/PDS 体系为有机废水处理提供了一种改进的有前景的高级氧化工艺。