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使用钴掺杂柚子皮碳复合材料活化过一硫酸盐对四环素进行氧化降解。

Oxidative degradation of tetracycline using peroxymonosulfate activated by cobalt-doped pomelo peel carbon composite.

机构信息

College of Forestry, Northeast Forestry University, Hexing Road 26, Harbin, 150040, China.

出版信息

Environ Sci Pollut Res Int. 2022 Mar;29(15):21656-21669. doi: 10.1007/s11356-021-17391-9. Epub 2021 Nov 12.

Abstract

Tetracycline (TC) is a typical ecotoxic antibiotic, which easily causes bacterial resistance. Therefore, it is necessary to remove TC from the water environment. In recent years, advanced oxidation processes (AOPs) rely on the use of highly reactive oxidizing sulfate radical which is turning into an increasingly popular as a tool of the removal of TC. In this study, cobalt-doped pomelo peel carbon composite (Co-PPCC) was prepared by the impregnation coprecipitation method to activate peroxymonosulfate (PMS) to remove TC. SEM, BET, XRD, FTIR, XPS, TGA, and other analytical techniques indicated that a carbon composite catalyst with excellent performance has been successfully prepared. TC was removed by the synergistic effect of adsorption and catalytic degradation processes. The adsorption capacity was limited (only approximately 20% within 60 min) and tending to saturation, which indicated that the removal of TC in the Co-PPCC/PMS system was mainly due to oxidative degradation. The influence of the Co-PPCC and PMS dosage, initial TC concentration, initial pH values, and coexisting anions on the removal efficiency of TC was investigated. When the Co-PPCC catalyst dosage was 1 g/L, PMS concentration was 2 g/L, and pH value was 11, the removal efficiency of TC with a concentration of 50 mg/L reached 99% within 60 min. Free radical quenching experiment and electron paramagnetic resonance (EPR) analysis indicated that the free radical and non-radical degradation processes exist in the Co-PPCC/PMS/TC system. The main degradation products and the possible transformation pathways of TC were explored by LC-MS. In addition, after four cycles of Co-PPCC tests, the removal efficiency of TC can reach 64%. This study provides a new method to reuse abandoned pomelo peels and synthesize an economical and environmentally friendly catalyst for activating peroxymonosulfate to remove TC antibiotics in water.

摘要

四环素(TC)是一种典型的生态毒性抗生素,容易引起细菌耐药性。因此,有必要从水环境中去除 TC。近年来,高级氧化工艺(AOPs)依赖于使用高反应性的硫酸根自由基,作为去除 TC 的工具,这种方法越来越受欢迎。本研究通过浸渍共沉淀法制备了柚子皮负载钴的碳复合材料(Co-PPCC),以激活过一硫酸盐(PMS)去除 TC。SEM、BET、XRD、FTIR、XPS、TGA 等分析技术表明,已成功制备出性能优异的碳复合材料催化剂。TC 的去除是通过吸附和催化降解过程的协同作用实现的。吸附容量有限(仅在 60 分钟内约为 20%),趋于饱和,这表明 Co-PPCC/PMS 体系中 TC 的去除主要是由于氧化降解。考察了 Co-PPCC 和 PMS 用量、初始 TC 浓度、初始 pH 值和共存阴离子对 TC 去除效率的影响。当 Co-PPCC 催化剂用量为 1 g/L、PMS 浓度为 2 g/L、pH 值为 11 时,浓度为 50 mg/L 的 TC 在 60 分钟内去除率达到 99%。自由基猝灭实验和电子顺磁共振(EPR)分析表明,Co-PPCC/PMS/TC 体系中存在自由基和非自由基降解过程。通过 LC-MS 探讨了 TC 的主要降解产物和可能的转化途径。此外,经过四次 Co-PPCC 测试后,TC 的去除效率可达 64%。本研究为废弃柚子皮的再利用提供了一种新方法,合成了一种经济环保的催化剂,用于激活过一硫酸盐去除水中的 TC 抗生素。

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