Electrochemical oxidation of sulfamethoxazole in BDD anode system: Degradation kinetics, mechanisms and toxicity evaluation

被引:101
作者
Hai, Hao [1 ]
Xing, Xuan [1 ]
Li, Si [2 ]
Xia, Shuhua [1 ]
Xia, Jianxin [1 ]
机构
[1] Minzu Univ China, Coll Life & Environm Sci, Dept Environm Sci, Beijing 100081, Peoples R China
[2] China Agr Univ, Coll Resources & Environm Sci, Beijing Key Lab Farmland Soil Pollut Prevent & Re, Beijing 100193, Peoples R China
基金
中国国家自然科学基金;
关键词
Electrochemical oxidation; Boron-doped diamond anode; Sulfamethoxazole; Degradation pathway; Toxicity analysis; ANTIBIOTIC TETRACYCLINE; ELECTRO-FENTON; WASTE-WATER; FLUOROQUINOLONE ANTIBIOTICS; REACTION PATHWAYS; RESISTANCE GENES; AQUEOUS-SOLUTION; REMOVAL; MINERALIZATION; PERFORMANCE;
D O I
10.1016/j.scitotenv.2020.139909
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
In the present study, electrochemical oxidation of sulfamethoxazole (SMX) with Boron-doped Diamond (BDD) anode and Stainless Steel (SS) cathode was investigated systematically. The effects of current density, initial pH, supporting electrolyte and natural organicmatter (NOM) onSMX degradation were explored. Under the conditions of current density 30 mA cm(-2), 0.1MNa(2)SO(4) used as supporting electrolyte, pH of 7 and without NOM affect, SMX was completely removed after 3 h electrolysis. COD removal efficiency, current efficiency and energy consumption were 65.6%, 40.1%, 72 kWh kg COD-1, respectively. Degradation mechanism was analyzed based on the active sites of SMX identified by density functional theory (DFT) calculation and intermediates analysis by HPLC-Q-TOF-MS/MS. Three possible degradation pathways were proposed, with the replacement of -NH2 at aromatic ring by -OH, the oxidation of -NH2 to -NO2 and the addition of -OH on isoxazole ring observed. The active sites detected in reaction matched the DFT calculation results exactly. The toxicity of intermediates produced during electrolysis process was evaluated by Escherichia coli experiment. Results showed that, after 2 h electrolysis, the inhibition ratio was decreased from the initial value of 22.8% to 10%, which has already achieved the safety boundary. After 4 h electrolysis, the toxicity was almost zero even with still 60% COD remained in the solution. This phenomenon demonstrated that the toxicity of SMX and its intermediate products was reduced significantly during electrolysis process. (c) 2020 Elsevier B.V. All rights reserved.
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页数:11
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