过硫酸盐活化方式对水厂二级出水中有机物和抗生素抗性基因的去除效能与机制

孙丽华; 梅筱禹; 高呈; 冯萃敏

doi:10.13205/j.hjgc.202209010

过硫酸盐活化方式对水厂二级出水中有机物和抗生素抗性基因的去除效能与机制

doi: 10.13205/j.hjgc.202209010

1. 北京建筑大学城市雨水系统与水环境教育部重点实验室, 北京 100044;
2. 北京建筑大学环境与能源工程学院, 北京 100044;
3. 北京市市政工程设计研究总院有限公司, 北京 100082

基金项目:

国家自然科学基金(52070011)

北京建筑大学市属高校基本科研业务费项目(X18025)

详细信息

作者简介:
孙丽华(1978-),女,博士,副教授,主要从事再生水处理技术及膜法水处理技术研究。sunlihuashd@163.com

通讯作者:
孙丽华(1978-),女,博士,副教授,主要从事再生水处理技术及膜法水处理技术研究。sunlihuashd@163.com

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出版历程
- 收稿日期: 2021-09-14
- 网络出版日期: 2022-11-09

MECHANISMS AND EFFICIENCY OF REMOVAL OF ORGANIC MATTER AND ANTIBIOTIC RESISTANCE GENES IN SECONDARY EFFLUENT OF WATARPLANTS BY DIFFERENT PERSULFATE ACTIVATION METHODS

1. Key Laboratory of Urban Rainwater System and Water Environment, Ministry of Education, Beijing University of Civil Engineering and Architecture, Beijing 100044, China;
2. School of Environmental and Energy Engineering, Beijing University of Civil Engineering and Architecture, Beijing 100044, China;
3. Beijing General Municipal Engineering Design & Research Institute Co., Ltd, Beijing 100082, China

摘要

摘要: 分别采用纳米零价铁(nZVI)和超声(US)技术对过硫酸盐(PS)进行活化,探究PS、nZVI/PS和US/PS 3种预氧化工艺对城市污水厂二级出水中不同类型抗生素抗性基因(antibiotic resistance genes, ARGs)和溶解性有机物(dissolved organic matter, DOC)的去除效能与机制。结果表明:最佳PS和nZVI投加量为4,2 mmol/L,US最佳功率为40 kHz,经过PS、nZVI/PS和US/PS预氧化反应后,二级出水中ARGs(tetA、tetC、sulⅠ、sulⅡ),intⅠ1及16S rRNA的浓度分别为10^4.38~10^6.82,10^4.02~10^5.97,10^4.02~10^6.98 copies/mL;在最佳反应条件下DOC去除率分别为11.2%、17.2%和15.3%;其中,nZVI/PS对ARGs和DOC的去除效果最好。3种预氧化过程中均有OH·和SO₄^-·参与反应,相较于PS和US/PS,nZVI/PS预氧化过程中产生的SO₄^-·和OH·含量最多,且SO₄^-·在反应体系中的浓度最高。因此,nZVI/PS预氧化方式可作为后续处理二级出水中ARGs和DOC的有效去除方法。
- 抗生素抗性基因 /
- 过硫酸盐 /
- 纳米零价铁 /
- 超声 /
- 自由基
Abstract: This paper used iron nanoparticles(nFe) and ultrasound(US) to activate persulfate(PS), then explored the removal efficiencies of PS, nFe/PS and US/PS in pre-oxidation processes on antibiotic resistance genes(ARGs) and dissolved organic matter(DOC) in secondary effluent, and discussed their removal mechanisms. The results showed that the optimal dosages of PS, nFe and US were determined to be 4 mmol/L, 2 mmol/L and 40 kHz, respectively. After PS, nFe/PS and US/PS pre-oxidation reactions, concentrations of ARGs(tetA, tetC, sulⅠ, sulⅡ), intⅠ1 and 16 S rRNA were 10^4.38~10^6.82, 10^4.02~10^5.97 and 10^4.02~10^6.98, respectively. Under the optimal reaction conditions, the removal rates of DOC were 11.2%, 17.2% and 15.3%, respectively. Among them, nFe/PS had the best removal effect on the above-mentioned ARGs and DOC. In the three pre-oxidation processes, OH· and SO₄^-· all participated in the reaction. Compared with PS alone and US/PS combined processes, the content of OH· and SO₄^-· generated was the highest in the pre-oxidation of nFe/PS, and the concentration of SO₄^-· was the highest in the reaction system. Therefore, the nFe/PS pre-oxidation method could be used as a subsequent treatment to effectively remove ARGs and DOC in the secondary effluent.
- antibiotic resistance genes /
- persulfate /
- nano-iron /
- ultrasound /
- free radicals

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参考文献(31)

[1]	BIROŠOVÁ L,MACKUL’AK T,BODÍK I,et al.Pilot study of seasonal occurrence and distribution of antibiotics and drug-resistant bacteria in wastewater treatment plants in Slovakia[J].Science of the Total Environment,2014,490:440-444.
[2]	罗义,周启星.抗生素抗性基因(ARGs):一种新型环境污染物[J].环境科学学报,2008,28(8):1499-1505.
[3]	DAVIES J,DAVIES D.Origins and evolution of antibiotic resistance[J].Microbiology and Molecular Biology Reviews,2010,74(3):417-433.
[4]	段然.哈尔滨市污水厂中抗生素抗性基因分布及强化去除研究[D].哈尔滨:哈尔滨工业大学,2014.
[5]	GARRIDO-CARDENAS J A,ESTEBAN-GARCÍA B,AGÜERA A,et al.Wastewater treatment by advanced oxidation process and their worldwide research trends[J].International Journal of Environmental Research and Public Health,2020,17(1):170.
[6]	李社锋,王文坦,邵雁,等.活化过硫酸盐高级氧化技术的研究进展及工程应用[J].环境工程,2016,34(9):171-174.
[7]	ANIPSITAKIS G P,DIONYSIOU D D.Radical generation by the interaction of transition metals with common oxidants[J].Environmental Science & Technology,2004,38(13):3705-3712.
[8]	AHMED M M,CHIRON S.Solar photo-Fenton like using persulphate for carbamazepine removal from domestic wastewater[J].Water Research,2014,48:229-236.
[9]	GIRI R R,OZAKI H,MORIGAKI T,et al.UV photolysis of perfluorooctanoic acid (PFOA) in dilute aqueous solution[J].Water Science and Technology,2011,63(2):276-282.
[10]	HUANG K C,ZHAO Z Q,HOAG G E,et al.Degradation of volatile organic compounds with thermally activated persulfate oxidation[J].Chemosphere,2005,61(4):551-560.
[11]	CHENG J,VECITIS C D,PARK H,et al.Sonochemical degradation of perfluorooctane sulfonate (PFOS) and perfluorooctanoate (PFOA) in landfill groundwater:environmental matrix effects[J].Environmental Science & Technology,2008,42(21):8057-8063.
[12]	MATZEK L W,CARTER K E.Activated persulfate for organic chemical degradation:a review[J].Chemosphere,2016,151:178-188.
[13]	ZHANG L L,JIN H,MA H K,et al.Oxidative damage of antibiotic resistant E.coli and gene in a novel sulfidated micron zero-valent activated persulfate system[J].Chemical Engineering Journal,2020,381:122787.
[14]	ZHANG B T,ZHANG Y,TENG Y G,et al.Sulfate radical and its application in decontamination technologies[J].Critical Reviews in Environmental Science and Technology,2015,45(16):1756-1800.
[15]	LI B Z,ZHU J.Simultaneous degradation of 1,1,1-trichloroethane and solvent stabilizer 1,4-dioxane by a sono-activated persulfate process[J].Chemical Engineering Journal,2016,284:750-763.
[16]	罗晓,袁立霞,郑向阳,等.制药废水中抗性基因和微生物群落相关性研究[J].环境科学与技术,2018,41(12):30-36 ,48.
[17]	OLMEZ-HANCI T,ARSLAN-ALATON I,GENC B.Bisphenol A treatment by the hot persulfate process:oxidation products and acute toxicity[J].Journal of Hazardous Materials,2013,263:283-290.
[18]	龙海波,高焕方,李聪,等.铁活化过硫酸盐修复石油烃污染土壤的研究进展[J].化工环保,2019,39(3):241-246.
[19]	李永涛,岳东,熊鑫高原,等.零价铁活化过硫酸钠降解含油废水[J].环境工程学报,2016,10(8):4239-4243.
[20]	张羽,高春阳,陈昌照,等.零价铁活化过硫酸钠体系降解污染土壤中的多环芳烃[J].环境工程学报,2019,13(4):955-962.
[21]	杨晴,孙昕,李鹏飞,等.超声活化过硫酸盐降解甲基橙的影响因素研究[J].环境科学学报,2020,40(8):2715-2721.
[22]	CHEN W S,HUANG C P.Mineralization of dinitrotoluenes in aqueous solution by sono-activated persulfate enhanced with electrolytes[J].Ultrasonics Sonochemistry,2019,51:129-137.
[23]	YAN W L,HERZING A A,KIELY C J,et al.Nanoscale zero-valent iron (nZVI):aspects of the core-shell structure and reactions with inorganic species in water[J].Journal of Contaminant Hydrology,2010,118(3/4):96-104.
[24]	何光瑞.超声零价铁活化过硫酸盐去除水中阿莫西林和卡马西平的研究[D].武汉:华中科技大学,2017.
[25]	O’CARROLL D,SLEEP B,KROL M,et al.Nanoscale zero valent iron and bimetallic particles for contaminated site remediation[J].Advances in Water Resources,2013,51:104-122.
[26]	ZHAO J Y,ZHANG Y B,QUAN X,et al.Enhanced oxidation of 4-chlorophenol using sulfate radicals generated from zero-valent iron and peroxydisulfate at ambient temperature[J].Separation and Purification Technology,2010,71(3):302-307.
[27]	MATTA R,TLILI S,CHIRON S,et al.Removal of carbamazepine from urban wastewater by sulfate radical oxidation[J].Environmental Chemistry Letters,2011,9(3):347-353.
[28]	XIA D H,YIN R,SUN J L,et al.Natural magnetic pyrrhotite as a high-Efficient persulfate activator for micropollutants degradation:radicals identification and toxicity evaluation[J].Journal of Hazardous Materials,2017,340:435-444.
[29]	WU Y W,CHEN X T,HAN Y,et al.Highly efficient utilization of nano-Fe (0) embedded in mesoporous carbon for activation of peroxydisulfate[J].Environmental Science & Technology,2019,53(15):9081-9090.
[30]	OH W D,DONG Z L,LIM T T.Generation of sulfate radical through heterogeneous catalysis for organic contaminants removal:current development,challenges and prospects[J].Applied Catalysis B:Environmental,2016,194:169-201.
[31]	沈阳.超声空化的理论研究及影响因素的模拟分析[D].沈阳:东北大学,2014.