常州大学 环境与安全工程学院,江苏 常州 213164
丁朋飞(1995- ),男,主要从事水处理技术研究,E-mail:ding19850239681@163.com。
郑璐(通信作者),女,博士,高级工程师,E-mail:zhenglu@cczu.edu.cn。
收稿:2021-06-20,
纸质出版:2023-12-25
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丁朋飞,陆金鑫,汤慧俐等.次氯酸钠对磺胺二甲氧嗪的降解与风险评价[J].土木与环境工程学报,2023,45(06):206-214.
DING Pengfei,LU Jinxin,TANG Huili,et al.Degradation and risk assessment of sulfadimethoxine during sodium hypochlorite disinfection process[J].Journal of Civil and Environmental Engineering,2023,45(06):206-214.
丁朋飞,陆金鑫,汤慧俐等.次氯酸钠对磺胺二甲氧嗪的降解与风险评价[J].土木与环境工程学报,2023,45(06):206-214. DOI: 10.11835/j.issn.2096-6717.2021.184.
DING Pengfei,LU Jinxin,TANG Huili,et al.Degradation and risk assessment of sulfadimethoxine during sodium hypochlorite disinfection process[J].Journal of Civil and Environmental Engineering,2023,45(06):206-214. DOI: 10.11835/j.issn.2096-6717.2021.184.
自来水原水中新兴污染物的存在对饮用水水质安全提出新的挑战。采用氯消毒对典型磺胺类抗生素磺胺二甲氧嗪(Sulfadimethoxine,SDM)进行降解研究,考察余氯初始浓度、pH值、氨氮(NH
4
-N)等因素对降解的影响,探究SDM氯氧化降解机理,评估其生态风险。结果表明:在SDM初始浓度为15 μmol/L、余氯初始浓度为60 μmol/L的条件下,120 s内SDM去除率达到95.9%,降解过程符合准二级反应动力学。反应速率常数随着余氯初始浓度增大而增大,随着NH
4
+
-N浓度增大而减小,背景阴离子Cl
-
、NO
3
-
、SO
4
2-
对反应影响甚微,HCO
3
-
、CO
3
2-
对反应有抑制作用,中性条件下有利于SDM氯氧化反应。基于高分辨质谱HRMS Orbitrap解析出9种降解中间产物,降解过程中发生氯代反应、脱甲基反应和羟基加成反应等。在消毒过程中,SDM的完全去除并不意味着生态风险的有效削减,对饮用水水质安全构成潜在风险。
The presence of emerging contaminants in the raw water puts forward new challenges to drinking water treatment process. The chlorination of typical sulfonamides antibiotic sulfadimethoxine (SDM) in the sodium hypochlorite disinfection process was studied. The chlorination effects
including the initial concentration of residual chlorine
the pH value of the solution
ammonia concentration
and the inorganic anions
were also investigated. The mechanism of SDM chlorination was explored and the ecological risk was further assessed. The results showed that
under the conditions of the initial SDM concentration 15 μmol/L
the initial concentration of residual chlorine 60 μmol/L
the SDM removal reached high up to 95.9% in 120 s. The degradation process conformed to the pseudo-second reaction kinetics. The constants of degradation rate decreased with the increasing ammonia concentration
and increased with the initial concentration of residual chlorine. Background anions Cl
-
NO
3-
SO
4
2-
had marginal effects on the reaction while HCO
3
-
and CO
3
2-
had inhibition effects on the reaction. SDM chlorination can be improved under neutral conditions. Nine degradation intermediates are identified by using high-resolution mass spectrometry HRMS Orbitrap. The degradation process covers chlorination
demethylation and hydroxyl addition reactions. The complete removal of SDM does not imply an effective reduction of ecological risk during disinfection process which poses a potential risk to the safety of drinking water quality.
CHOKEJAROENRAT C , SAKULTHAEW C , ANGKAEW A , et al . Remediating sulfadimethoxine-contaminated aquaculture wastewater using ZVI-activated persulfate in a flow-through system [J]. Aquacultural Engineering , 2019 , 84 : 99 - 105 .
WANG Z , ZHANG X H , HUANG Y , et al . Comprehensive evaluation of pharmaceuticals and personal care products (PPCPs) in typical highly urbanized regions across China [J]. Environmental Pollution , 2015 , 204 : 223 - 232 .
KÜMMERER K . Antibiotics in the aquatic environment- A review - Part I [J]. Chemosphere , 2009 , 75 ( 4 ): 417 - 434 .
KÜMMERER K . Antibiotics in the aquatic environment- A review-Part II [J]. Chemosphere , 2009 , 75 ( 4 ): 435 - 441 .
XIN X D , SUN S H , ZHOU A R , et al . Sulfadimethoxine photodegradation in UV-C/H 2 O 2 system: Reaction kinetics, degradation pathways, and toxicity [J]. Journal of Water Process Engineering , 2020 , 36 : 101293 .
王小宁 , 杨传玺 , 宗万松 . 饮用水消毒副产物生物毒性与调控策略的研究 [J]. 工业水处理 , 2017 , 37 ( 1 ): 12 - 17 .
WANG X N , YANG C X , ZONG W S . Research on biological toxicity of drinking water disinfection by-products and its control strategies [J]. Industrial Water Treatment , 2017 , 37 ( 1 ): 12 - 17 . (in Chinese)
LI L P . Toxicity evaluation and by-products identification of triclosan ozonation and chlorination [J]. Chemosphere , 2021 , 263 : 128223 .
DE BARROS A L C , SILVA RODRIGUES D ADA , CUNHA C C R FDA , et al . Aqueous chlorination of herbicide metribuzin: Identification and elucidation of “new” disinfection by-products, degradation pathway and toxicity evaluation [J]. Water Research , 2021 , 189 : 116545 .
ADAMS C , WANG Y , LOFTIN K , et al . Removal of antibiotics from surface and distilled water in conventional water treatment processes [J]. Journal of Environmental Engineering , 2002 , 128 ( 3 ): 253 - 260 .
SAPOZHNIKOVA Y , HEDGESPETH M , WIRTH E , et al . Analysis of selected natural and synthetic hormones by LC-MS-MS using the US EPA method 1694 [J]. Analytical Methods , 2011 , 3 ( 5 ): 1079 .
CHEN J , XU X X , ZENG X L , et al . Ferrate(VI) oxidation of polychlorinated diphenyl sulfides: Kinetics, degradation, and oxidized products [J]. Water Research , 2018 , 143 : 1 - 9 .
严静娜 , 张小寒 , 任源 . 次氯酸钠氧化消除水中双氯芬酸的动力学及影响因素 [J]. 水处理技术 , 2017 , 43 ( 9 ): 56 - 61, 66 .
YAN J N , ZHANG X H , REN Y . Kinetic and influencing factors of diclofenac oxidation in water by sodium hypochlorite [J]. Technology of Water Treatment , 2017 , 43 ( 9 ): 56 - 61, 66 . (in Chinese)
ACERO J L , PIRIOU P , VON GUNTEN U . Kinetics and mechanisms of formation of bromophenols during drinking water chlorination: Assessment of taste and odor development [J]. Water Research , 2005 , 39 ( 13 ): 2979 - 2993 .
ACERO J L , REAL F J , BENITEZ F J , et al . Kinetics of reactions between chlorine or bromine and the herbicides diuron and isoproturon [J]. Journal of Chemical Technology & Biotechnology , 2007 , 82 ( 2 ): 214 - 222 .
DING J Q , NIE H , WANG S L , et al . Transformation of acetaminophen in solution containing both peroxymonosulfate and chlorine: Performance, mechanism, and disinfection by-product formation [J]. Water Research , 2021 , 189 : 116605 .
XIANG W R , CHANG J Y , QU R J , et al . Transformation of bromophenols by aqueous chlorination and exploration of main reaction mechanisms [J]. Chemosphere , 2021 , 265 : 129112 .
李军 , 葛林科 , 张蓬 , 等 . 磺胺类抗生素在水环境中的光化学行为 [J]. 环境化学 , 2016 , 35 ( 4 ): 666 - 679 .
LI J , GE L K , ZHANG P , et al . Progress in studies on photochemical behavior of sulfonamide antibiotics in aquatic environment [J]. Environmental Chemistry , 2016 , 35 ( 4 ): 666 - 679 . (in Chinese)
闫淑霞 , 刘春花 , 梁岩 . 腐殖酸的结构特性与应用研究进展 [J]. 天然产物研究与开发 , 2017 , 29 ( 3 ): 511 - 516 .
YAN S X , LIU C H , LIANG Y . Review on structural properties and multiple functionalities of humic acids [J]. Natural Product Research and Development , 2017 , 29 ( 3 ): 511 - 516 . (in Chinese)
程艳 , 陈会明 , 于文莲 , 等 . QSAR技术对高关注化学物质生态环境毒理风险预测 [J]. 环境科学研究 , 2009 , 22 ( 7 ): 817 - 822 .
CHENG Y , CHEN H M , YU W L , et al . Eco-environmental toxicity risk prediction for substances of very high concern with QSAR approach [J]. Research of Environmental Sciences , 2009 , 22 ( 7 ): 817 - 822 . (in Chinese)
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