College of Environmental Science and Engineering, Hunan University, Changsha, Hunan 410082, China; Key Laboratory of Environmental Biology and Pollution Control (Hunan University), Ministry of Education, Changsha, Hunan 410082, China.
College of Environmental Science and Engineering, Hunan University, Changsha, Hunan 410082, China; Key Laboratory of Environmental Biology and Pollution Control (Hunan University), Ministry of Education, Changsha, Hunan 410082, China.
J Hazard Mater. 2022 Aug 5;435:128999. doi: 10.1016/j.jhazmat.2022.128999. Epub 2022 Apr 23.
This work presents a novel CuS/percarbonate/tetraacetylethylenediamine (CuS/SPC/TAED) process for the degradation of sulfamethazine (SMT). Results indicated that the CuS/SPC/TAED process enabled the efficient generation of peracetic acid (PAA), which can be efficiently activated by CuS in alkaline reaction media, and 93.6% of SMT was degraded in 30 min. Mechanism study revealed that the available reactive oxygen species (ROS) including hydroxyl radical (OH), carbonate radical (CO), superoxide radical (O), singlet oxygen (O), and organic radicals (R-O). Among them, R-O (acetyloxyl radical (CHCO) and acetylperoxyl radical (CHCO)) were confirmed to be the primary species that contributed to SMT degradation. Simultaneously, the role of sulfur species and carbonate ions were explored. It was found that the reductive O and sulfur species rendered the efficient redox of Cu species. Besides, the effects of key influencing factors including SPC/TAED mole ratio, CuS dosage, initial pH, temperature, and nontarget matrix constituents on SMT degradation were examined. Finally, the degradation intermediates of SMT was identified, and the toxicity of these products was estimated by quantitative structure-activity relationship (QSAR) analysis. Overall, this work offers a new and simple strategy for antibiotic-polluted water remediation.
本工作提出了一种新颖的 CuS/过碳酸盐/四乙酰乙二胺(CuS/SPC/TAED)工艺,用于降解磺胺甲噁唑(SMT)。结果表明,CuS/SPC/TAED 工艺能够有效地生成过氧乙酸(PAA),在碱性反应介质中,CuS 可以有效地激活 PAA,在 30 分钟内,93.6%的 SMT 被降解。机理研究表明,包括羟基自由基(OH)、碳酸根自由基(CO)、超氧自由基(O)、单线态氧(O)和有机自由基(R-O)在内的活性氧物质(ROS)可被有效生成。其中,R-O(乙酰氧基自由基(CHCO)和乙酰过氧自由基(CHCO))被证实是导致 SMT 降解的主要物质。同时,还研究了硫物种和碳酸根离子的作用。结果发现,还原态 O 和硫物种使 Cu 物种的有效氧化还原。此外,还考察了 SPC/TAED 摩尔比、CuS 用量、初始 pH 值、温度和非目标基质成分等关键影响因素对 SMT 降解的影响。最后,鉴定了 SMT 的降解中间产物,并通过定量结构-活性关系(QSAR)分析评估了这些产物的毒性。总体而言,本工作为抗生素污染水的修复提供了一种新的简单策略。