活化过硫酸盐杀灭水中大肠杆菌
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摘要
通过亚铁离子(Fe~(2+))活化过硫酸氢钾(PMS)产生硫酸根自由基(SO_4~-·),从而杀灭水中大肠杆菌。分析未活化的PMS、亚铁离子浓度、初始pH值、络合剂种类及浓度等因素对系统杀灭水中大肠杆菌效果的影响,并简要分析其杀菌机理。结果表明,未活化的PMS对水中大肠杆菌的杀灭能力有限,当PMS浓度为1 mmol/L时,对大肠杆菌的对数去除率仅为1. 4-lg;加入适量亚铁离子能显著提高杀灭效果,当PMS和Fe~(2+)的浓度均为0. 3 mmol/L时,对大肠杆菌的对数去除率达到6. 3-lg,而亚铁离子过量时则产生抑制效果;系统初始pH值对大肠杆菌的杀灭效果有显著影响,对数去除率随着pH值的升高而降低;在PMS/Fe~(2+)体系中加入柠檬酸及EDTA均可产生抑制效果,加入适量焦磷酸钾则具有促进作用。硫酸根自由基首先破坏细胞结构,使细胞膜破裂,进而对其内容物进行氧化破坏,导致细胞死亡。
Escherichia coli (E. coli) in water was killed by sulfate radicals (SO_4~-·) produced by potassium peroxymonosulfate (PMS) activated by ferrous ions (Fe~(2+)). The influences of unactivated PMS,Fe~(2+) concentration,initial pH value,types and concentration of different complexants on killing efficacy were explored,and the sterilizing mechanism was briefly analyzed. The results showed that the unactivated PMS had limited ability to kill E. coli. When the concentration of PMS was 1 mmol/L,the logarithm removal rate of E. coli was only 1. 4-lg. When a proper amount of Fe~(2+)was added,the sterilization effect of E. coli was significantly increased. When concentrations of PMS and Fe~(2+) were both 0. 3 mmol/L,the logarithm removal rate reached 6. 3-lg. However,excess Fe~(2+) would inhibit the sterilization effect. The initial pH value of the system had a significant influence on the sterilization effect,and the logarithm removal rate decreased with the increase of pH value. The addition of citric acid or EDTA in the PMS/Fe~(2+)system would both lead to inhibitory effect, while the addition of a proper amount of potassium pyrophosphate would promote the sterilization effect. Sulfate radical first destroyed the cell structure which led to cell membrane rupture. Then, cellular contents were oxidized and destroyed which eventually resulted in cell death.
Escherichia coli (E. coli) in water was killed by sulfate radicals (SO_4~-·) produced by potassium peroxymonosulfate (PMS) activated by ferrous ions (Fe~(2+)). The influences of unactivated PMS,Fe~(2+) concentration,initial pH value,types and concentration of different complexants on killing efficacy were explored,and the sterilizing mechanism was briefly analyzed. The results showed that the unactivated PMS had limited ability to kill E. coli. When the concentration of PMS was 1 mmol/L,the logarithm removal rate of E. coli was only 1. 4-lg. When a proper amount of Fe~(2+)was added,the sterilization effect of E. coli was significantly increased. When concentrations of PMS and Fe~(2+) were both 0. 3 mmol/L,the logarithm removal rate reached 6. 3-lg. However,excess Fe~(2+) would inhibit the sterilization effect. The initial pH value of the system had a significant influence on the sterilization effect,and the logarithm removal rate decreased with the increase of pH value. The addition of citric acid or EDTA in the PMS/Fe~(2+)system would both lead to inhibitory effect, while the addition of a proper amount of potassium pyrophosphate would promote the sterilization effect. Sulfate radical first destroyed the cell structure which led to cell membrane rupture. Then, cellular contents were oxidized and destroyed which eventually resulted in cell death.
引文
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[4]Rizzo L,Manaia C,Merlin C,et al.Urban wastewater treatment plants as hotspots for antibiotic resistant bacteria and genes spread into the environment:A review[J].Sci Total Environ,2013,447:345-360.
[5]Yuan S,Liao P,Alshawabkeh A N.Electrolytic manipulation of persulfate reactivity by iron electrodes for trichloroethylene degradation in groundwater[J].Environ Sci Technol,2014,48(1):656-663.
[6]Chesney A R,Booth C J,Lietz C B,et al.Peroxymonosulfate rapidly inactivates the disease-associated prion protein[J].Environ Sci Technol,2016,50(13):7095-7105.
[7]Wang J L,Wang S Z.Activation of persulfate(PS)and peroxymonosulfate(PMS)and application for the degradation of emerging contaminants[J].Chem Eng J,2018,334:1502-1517.
[8]李若白,刘国光,吕文英,等.Fe2+活化过硫酸氢钾复合盐降解吲哚美辛[J].环境工程学报,2016,10(10):5429-5432.Li Ruobai,Liu Guoguang,LüWenying,et al.Degradation of indomethacin in aqueous by peroxymonosulfate activated by ferrous ion[J].Chinese Journal of Environmental Engineering,2016,10(10):5429-5432(in Chinese).
[9]张利朋,王枫亮,陈平,等.亚铁离子活化过硫酸氢钾复合盐降解水溶液中酮洛芬[J].环境工程学报,2017,11(2):847-851.Zhang Lipeng,Wang Fengliang,Chen Ping,et al.Degradation of ketoprofen in aqueous by peroxymonosulfate actived by ferrous ion[J].Chinese Journal of Environmental Engineering,2017,11(2):847-851(in Chinese).
[10]Huang Y F,Huang Y H.Identification of produced powerful radicals involved in the mineralization of bisphenol Ausing a novel UV-Na2S2O8/H2O2-Fe(Ⅱ,Ⅲ)two-stage oxidation process[J].J Hazard Mater,2009,162(2/3):1211-1216.
[11]张成,万金泉,马邕文,等.p H及络合剂对亚铁活化S2O2-8氧化去除活性艳蓝的影响研究[J].环境科学,2012,33(3):871-878.Zhang Cheng,Wan Jinquan,Ma Yongwen,et al.Influences of p H and complexing agents on degradation of reactive brilliant blue KN-R by ferrous activated persulfate[J].Environmental Science,2012,33(3):871-878(in Chinese).
[12]张利朋.亚铁离子活化过硫酸氢钾复合盐降解水溶液中酮洛芬的研究[D].广州:广东工业大学,2016.Zhang Lipeng.Study on Degradation of Ketoprofen by Peroxymonosulfate Activated by Ferrous Ions[D].Guangzhou:Guangdong University of Technology,2016(in Chinese).
[13]韩东晖.基于有机酸络合铁离子活化过硫酸盐技术氧化降解有机污染物的研究[D].广州:华南理工大学,2015.Han Donghui.Study on the Persulfate Oxidation of Organic Contaminants Activated by Organic Acid Chelated Iron Ions[D].Guangzhou:South China University of Technology,2015(in Chinese).
[14]Cho M,Kim J,Kim J Y,et al.Mechanisms of Escherichia coli inactivation by several disinfectants[J].Water Res,2010,44(11):3410-3418.