Degradation of sulfamethoxazole by heat-activated persulfate oxidation: Elucidation of the degradation mechanism and influence of process parameters

被引:113
作者
Milh, Hannah [1 ]
Schoenaers, Ben [2 ]
Stesmans, Andre [2 ]
Cabooter, Deirdre [3 ]
Dewil, Raf [1 ]
机构
[1] Katholieke Univ Leuven, Proc & Environm Technol Lab, Dept Chem Engn, J De Nayerlaan 5, B-2860 St Katelijne Waver, Belgium
[2] Katholieke Univ Leuven, Lab Semicond Phys, Dept Phys & Astron, Celestijnenlaan 2004, B-3001 Leuven, Belgium
[3] Katholieke Univ Leuven, Lab Pharmaceut Anal, Dept Pharmaceut & Pharmacol Sci, Herestr 49, B-3000 Leuven, Belgium
关键词
Sulfamethoxazole; Heat-activated persulfate oxidation; SR-AOP; Degradation mechanism; Toxicity evaluation; PHENAZONE-TYPE PHARMACEUTICALS; HIGH-RESOLUTION MS; HYDROXYL RADICALS; PRODUCTS; GENERATION; TECHNOLOGIES; CONTAMINANTS; KINETICS; ATRAZINE; REMOVAL;
D O I
10.1016/j.cej.2019.122234
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
In this article, heat-activated persulfate oxidation was investigated as a promising technique for the removal of sulfamethoxazole from an aqueous environment. It was found that the degradation efficiency of sulfamethoxazole increases with increasing persulfate concentration due to the increased center dot SO(4)(- )production. As suggested by the Arrhenius equation, the sulfamethoxazole degradation rate constant increased with increasing temperature. An activation energy of 103 kJ/mol was determined. Furthermore, the initial pH of the reaction mixture had a large influence on the degradation of sulfamethoxazole. At higher initial pH values, the degradation of sulfamethoxazole increased. The main cause for this increase is a difference in sulfamethoxazole distribution: at higher pH, the deprotonated form of sulfamethoxazole is present and found to be more susceptible to degradation. A second reason was found to be the formation of center dot OH at higher initial pH values, although this contribution was smaller. To elucidate the degradation process, six intermediates were identified, and the difference in formation of these compounds at different initial pH values was revealed. Through ECOSAR modeling, some degradation products were found to be of main interest when monitoring the toxicity of the degradation mixture.
引用
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页数:12
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