氧化还原介体强化高铁酸盐降解新污染物

宋利先, 郑成志, 于永强, 张静, 马军

中国环境科学 ›› 2024, Vol. 44 ›› Issue (8) : 4588-4598.

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PDF(2456 KB)
中国环境科学 ›› 2024, Vol. 44 ›› Issue (8) : 4588-4598.
美丽中国建设:新污染物

氧化还原介体强化高铁酸盐降解新污染物

  • 宋利先1, 郑成志2, 于永强1, 张静1, 马军1
作者信息 +

Redox mediator-enhancing ferrate(VI) oxidation of emerging contaminants

  • SONG Li-xian1, ZHENG Cheng-zhi2, YU Yong-qiang1, ZHANG Jing1, MA Jun1
Author information +
文章历史 +

摘要

以最具有代表性的氧化还原介体——四甲基哌啶氧化物(TEMPO)为研究对象,探究其强化高铁酸盐(Fe(VI))降新污染物的效能与作用机制.结果表明,该体系可在120s内对于磺胺甲恶唑(5μmol/L) 的去除效率达到73 %,通过深入分析,发现TEMPO+和Fe(V)/Fe(IV)是反应过程中的关键活性物种.同时对TEMPO浓度、初始pH值以及实际水体中常见组分(腐殖酸、无机阴离子)对反应体系的影响进行考察.由于均相催化剂回收利用困难且可能引发二次污染,进一步开发了4-氨基-TEMPO@SiO2非均相催化剂,所制备非均相催化剂对于酚类、沙星类、四环素类污染物均表现出显著的强化效果,其中对苯酚和四环素的强化效果最好,可在20s内将其完全去除.

Abstract

The most representative redox mediator, tetramethylpyrazine oxide (TEMPO), was used to investigate the efficacy and mechanism of its enhanced degradation of emerging contaminants by ferrate (Fe(VI)). The results showed that the system could remove 73% of sulfamethoxazole (5μmol/L) within 120 seconds. Through in-depth analysis, it was found that TEMPO+ and Fe(V)/Fe(IV) are key active species in the system. Additionally, the effects of TEMPO concentration, initial pH and common components (humic acid, inorganic anions) in the actual water on the reaction system were investigated. Given the difficulties in recycling and potential secondary pollution of homogeneous catalysts, the 4-amino-TEMPO@SiO2 heterogeneous catalysts were further developed. The prepared heterogeneous catalyst demonstrated significant enhancement effects on phenolic, quinolone, and tetracycline pollutants, with the most notable effects on phenol and tetracycline, which can be completely removed in just 20 seconds.

关键词

动力学 / 反应性物种 / 高铁酸盐 / 四甲基哌啶氧化物 / 新污染物

Key words

emerging contaminants / ferrate / kinetics / oxidizing species / tetramethylpiperidine oxides

引用本文

导出引用
宋利先, 郑成志, 于永强, 张静, 马军. 氧化还原介体强化高铁酸盐降解新污染物[J]. 中国环境科学. 2024, 44(8): 4588-4598
SONG Li-xian, ZHENG Cheng-zhi, YU Yong-qiang, ZHANG Jing, MA Jun. Redox mediator-enhancing ferrate(VI) oxidation of emerging contaminants[J]. China Environmental Science. 2024, 44(8): 4588-4598
中图分类号: X703   

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国家自然科学基金面上项目(22076016)

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