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氧化还原介体强化高铁酸盐降解新污染物

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

tetramethylpiperidine oxidesferrateemerging contaminantskineticsoxidizing species

宋利先、郑成志、于永强、张静、马军

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哈尔滨工业大学环境学院,城市水资源与水环境国家重点实验室,黑龙江哈尔滨 150000

哈尔滨工业大学水资源国家工程研究中心有限公司,黑龙江哈尔滨 150000

四甲基哌啶氧化物 高铁酸盐 新污染物 动力学 反应性物种

国家自然科学基金面上项目

22076016

2024

中国环境科学
中国环境科学学会

中国环境科学

CSTPCDCHSSCD北大核心
影响因子:2.174
ISSN:1000-6923
年,卷(期):2024.44(8)