Nonradical transformation of sulfamethoxazole by carbon nanotube activated peroxydisulfate: Kinetics, mechanism and product toxicity

被引:78
|
作者
Guan, Chaoting [1 ,2 ,4 ,5 ]
Jiang, Jin [1 ,2 ]
Pang, Suyan [3 ]
Ma, Jun [2 ]
Chen, Xiao [4 ,5 ]
Lim, Teik-Thye [4 ,5 ]
机构
[1] Guangdong Univ Technol, Inst Environm & Ecol Engn, Guangzhou 510006, Guangdong, Peoples R China
[2] Harbin Inst Technol, State Key Lab Urban Water Resource & Environm, Harbin 150090, Heilongjiang, Peoples R China
[3] Jilin Jianzhu Univ, Sch Municipal & Environm Engn, Minist Educ, Key Lab Songliao Aquat Environm, Changchun 130118, Jilin, Peoples R China
[4] Nanyang Technol Univ, NEWRI, Environm Chem & Mat Ctr, 1 Cleantech Loop,CleanTech One,06-08, Singapore 637141, Singapore
[5] Nanyang Technol Univ, Sch Civil & Environm Engn, 50 Nanyang Ave, Singapore 639798, Singapore
基金
中国国家自然科学基金;
关键词
Peroxydisulfate; Carbon nanotubes; Sulfamethoxazole; Nonradical oxidation; Transformation products; SYNTHETIC HUMAN URINE; ANTIBIOTIC SULFAMETHOXAZOLE; PERSULFATE OXIDATION; ORGANIC CONTAMINANTS; CATALYTIC-OXIDATION; DEGRADATION; PEROXYMONOSULFATE; PHARMACEUTICALS; GENERATION; CHLORINE;
D O I
10.1016/j.cej.2019.122147
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 work, the transformation of sulfamethoxazole (SMX) by peroxydisulfate (PDS) activated with one multiwalled carbon nanotube (CNT) via a nonradical pathway was examined, and the underlying reaction mechanism was explicated. The nonradical PDS/ CNT process exhibited considerable reactivity toward SMX, and the oxidation of SMX was enhanced by the decrease of solution pH. The addition of background inorganic ions (i.e., bicarbonate and chloride ion) showed ignorable impacts on SMX transformation, while natural organic matter resulted in the decrease of SMX oxidation rate. The stoichiometric efficiency of SMX degraded vs PDS consumed in the presence of CNT was obviously higher compared to that obtained in the case of zero-valent iron (a common heterogeneous metal activator for PDS). The oxidation of sub-structural model compounds in the PDS/CNT process unveiled that the main reactive functional group of SMX molecule for attack by nonradical reactive species was aniline moiety, while the isoxazole moiety could also be slowly oxidized. A total of six oxidation products were identified during SMX treatment by the PDS/CNT process, and their generation pathways mainly included hydroxylation, isoxazole ring opening, and sulfonamide NeS bond cleavage. Ecotoxicity analysis by ECOSAR showed that the toxicity of these products was generally lower than parent SMX. Consequently, this work demonstrate that the emerging PDS/CNT oxidation technology is likely a prospective candidate for destruction of SMX in water and wastewaters.
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页数:8
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