紫外/亚硫酸钠还原降解三氯乙酰胺的效能
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摘要
卤乙酰胺(HAc Ams)是一类具有高细胞毒性和高遗传毒性的饮用水含氮消毒副产物(N-DBPs),并在饮用水中被广泛检出,其中三氯乙酰胺(TCAc Am)的毒性显著高于传统DBPs.本实验以配置的TCAc Am溶液作为目标污染物,采用紫外(UV)活化亚硫酸钠(Na_2SO_3)体系降解水中的TCAc Am,并探究在该体系下光强、还原剂投加剂量(Na_2SO_3)和p H对还原降解TCAc Am效果的影响.结果表明,采用UV/Na_2SO_3体系可快速降解TCAc Am,其降解效果与光强、Na_2SO_3投加剂量和p H均呈正相关,且p H值对反应速率与降解率有显著影响,当p H值从6提高至9,TCAc Am的降解率在反应120 min时从12. 8%提高至99. 6%.在光强为450μW·cm~(-2),p H为9,Na_2SO_3投加剂量为1. 00 mmol·L~(-1),连续30 min光照条件下,TCAc Am降解率达到99. 4%.实验证明UV/Na_2SO_3体系是一种有效消减TCAc Am的高级还原技术,并且具备还原降解其他卤代DBPs的潜力,可用于饮用水中卤代DBPs的降解.
Haloacetamides( HAc Ams) are an emerging class of nitrogenous disinfection by-products( N-DBPs) with high cytotoxicity and genotoxicity,which are widely detected in drinking water. The toxicity of trichloroacetamide( TCAc Am) is significantly higher than traditional DBPs. In this study,ultraviolet( UV) treatment was combined with sodium sulphite( Na_2SO_3) to remove TCAc Am from water. The effects of different light intensities,different agent dosages( Na_2SO_3),and p H conditions on the removal of TCAc Am by UV/Na_2SO_3 advanced reduction process were investigated. The results showed that TCAc Am could be rapidly degraded by the UV/Na_2SO_3 system. The degradation effect was directly proportional to light intensity,dosage of Na_2SO_3,and p H. Moreover,the p H had a significant effect on the reaction rate and degradation rate. As the p H increased from 6 to 9,the degradation rate of TCAc Am increased from 12. 8% to 99. 6%,in 120 min. The removal rate of TCAc Am reached 99. 4% when the UV light intensity,p H,Na_2SO_3 dosage,and reaction time were 450 μW·cm~(-2),9,1. 00 mmol·L~(-1),and 30 min,respectively. The experimental results indicated that the UV/Na_2SO_3 system is an efficient advanced reduction process for the removal of TCAc Am,and it has the potential to reduce other halogenated DBPs. Therefore,it could be used for the degradation of halogenated DBPs in the treatment of drinking water.
Haloacetamides( HAc Ams) are an emerging class of nitrogenous disinfection by-products( N-DBPs) with high cytotoxicity and genotoxicity,which are widely detected in drinking water. The toxicity of trichloroacetamide( TCAc Am) is significantly higher than traditional DBPs. In this study,ultraviolet( UV) treatment was combined with sodium sulphite( Na_2SO_3) to remove TCAc Am from water. The effects of different light intensities,different agent dosages( Na_2SO_3),and p H conditions on the removal of TCAc Am by UV/Na_2SO_3 advanced reduction process were investigated. The results showed that TCAc Am could be rapidly degraded by the UV/Na_2SO_3 system. The degradation effect was directly proportional to light intensity,dosage of Na_2SO_3,and p H. Moreover,the p H had a significant effect on the reaction rate and degradation rate. As the p H increased from 6 to 9,the degradation rate of TCAc Am increased from 12. 8% to 99. 6%,in 120 min. The removal rate of TCAc Am reached 99. 4% when the UV light intensity,p H,Na_2SO_3 dosage,and reaction time were 450 μW·cm~(-2),9,1. 00 mmol·L~(-1),and 30 min,respectively. The experimental results indicated that the UV/Na_2SO_3 system is an efficient advanced reduction process for the removal of TCAc Am,and it has the potential to reduce other halogenated DBPs. Therefore,it could be used for the degradation of halogenated DBPs in the treatment of drinking water.
引文
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[13]Kosaka K,Ohkubo K,Akiba M.Occurrence and formation of haloacetamides from chlorination at water purification plants across Japan[J].Water Research,2016,106:470-476.
[14]Zhang Y,Zhang Z Y,Zhao Y P,et al.Identifying health effects of exposure to trichloroacetamide using transcriptomics and metabonomics in mice(Mus musculus)[J].Environmental Science&Technology,2013,47(6):2918-2924.
[15]杨世迎,张宜涛,郑迪.高级还原技术:一种水处理新技术[J].化学进展,2016,28(6):934-941.Yang S Y,Zhang Y T,Zheng D.Advanced reduction processes:a novel technology for water treatment[J].Progress in Chemistry,2016,28(6):934-941.
[16]Yu H,Nie E,Xu J,et al.Degradation of diclofenac by advanced oxidation and reduction processes:kinetic studies,degradation pathways and toxicity assessments[J].Water Research,2013,47(5):1909-1918.
[17]Li X C,Ma J,Liu G F,et al.Efficient reductive dechlorination of monochloroacetic acid by sulfite/UV process[J].Environmental Science&Technology,2012,46(13):7342-7349.
[18]Liu X,Vellanki B P,Batchelor B,et al.Degradation of 1,2-dichloroethane with advanced reduction processes(ARPs):effects of process variables and mechanisms[J].Chemical Engineering Journal,2014,237:300-307.
[19]Kaushik V,Duan Y H,Jung B,et al.Arsenic removal using advanced reduction process with dithionite/UV-A kinetic study[J].Journal of Water Process Engineering,2018,23:314-319.
[20]Yazdanbakhsh A,Eslami A,Moussavi G,et al.Photo-assisted degradation of 2,4,6-trichlorophenol by an advanced reduction process based on sulfite anion radical:degradation,dechlorination and mineralization[J].Chemosphere,2018,191:156-165.
[21]Vellanki B P,Batchelor B,Abdel-Wahab A.Advanced reduction processes:a new class of treatment processes[J].Environmental Engineering Science,2013,30(5):264-271.
[22]韩慧丽,王宏杰,董文艺.真空紫外-亚硫酸盐法降解PFOS影响因素[J].环境科学,2017,38(4):1477-1482.Han H L,Wang H J,Dong W Y.Influencing factors on the degradation of PFOS through VUV-SO2-3[J].Environmental Science,2017,38(4):1477-1482.
[23]Chu W H,Ding S K,Bond T,et al.Zero valent iron produces dichloroacetamide from chloramphenicol antibiotics in the absence of chlorine and chloramines[J].Water Research,2016,104:254-261.
[24]Gu Y,Dong W,Luo C,et al.Efficient reductive decomposition of perfluorooctanesulfonate in a high photon flux UV/sulfite system[J].Environmental Science&Technology,2016,50(19):10554-10561.
[25]Li X C,Fang J Y,Liu G F,et al.Kinetics and efficiency of the hydrated electron-induced dehalogenation by the sulfite/UVprocess[J].Water Research,2014,62:220-228.
[26]Xiao Q,Ren Y F,Yu S L.Pilot study on bromate reduction from drinking water by UV/sulfite systems:economic cost comparisons,effects of environmental parameters and mechanisms[J].Chemical Engineering Journal,2017,330:1203-1210.
[27]Liu X,Yoon S,Batchelor B,et al.Degradation of vinyl chloride(VC)by the sulfite/UV advanced reduction process(ARP):effects of process variables and a kinetic model[J].Science of the Total Environment,2013,454-455:578-583.
[28]Liu X W,Zhang T Q,Shao Y.Aqueous bromate reduction by UV activation of sulfite[J].CLEAN-Soil,Air,Water,2014,42(10):1370-1375.
[29]Xie B H,Li X C,Huang X F,et al.Enhanced debromination of4-bromophenol by the UV/sulfite process:Efficiency and mechanism[J].Journal of Environmental Sciences,2017,54:231-238.
[30]Song Z,Tang H Q,Wang N,et al.Reductive defluorination of perfluorooctanoic acid by hydrated electrons in a sulfite-mediated UV photochemical system[J].Journal of Hazardous Materials,2013,262:332-338.
[31]Liu X,Yoon S,Batchelor B,et al.Photochemical degradation of vinyl chloride with an advanced reduction process(ARP)-effects of reagents and pH[J].Chemical Engineering Journal,2013,215-216:868-875.
[32]Vellanki B P,Batchelor B.Perchlorate reduction by the sulfite/ultraviolet light advanced reduction process[J].Journal of Hazardous Materials,2013,262:348-356.
[33]Chu W H,Gao N Y,Deng Y.Stability of newfound nitrogenous disinfection by-products haloacetamides in drinking water[J].Chinese Journal of Organic Chemistry,2009,29(10):1569-1574.
[34]Ding S K,Wang F F,Chu W H,et al.Rapid degradation of brominated and iodinated haloacetamides with sulfite in drinking water:degradation kinetics and mechanisms[J].Water Research,2018,143:325-333.
[2]王尧,叶素红,章大山.Q市给水系统中消毒副产物的变化研究[J].中国给水排水,2018,34(9):44-46.Wang Y,Ye S H,Zhang D S.Variation of disinfection byproducts in domestic drinking water in Q City[J].China Water and Wastewater,2018,34(9):44-46.
[3]Chu W H,Gao N Y,Krasner S W,et al.Formation of halogenated C-,N-DBPs from chlor(am)ination and UVirradiation of tyrosine in drinking water[J].Environmental Pollution,2012,161:8-14.
[4]Bond T,Huang J,Templeton M R,et al.Occurrence and control of nitrogenous disinfection by-products in drinking water-Areview[J].Water Research,2011,45(15):4341-4354.
[5]Chu W H,Gao N Y,Deng Y,et al.Formation of nitrogenous disinfection by-products from pre-chloramination[J].Chemosphere,2011,85(7):1187-1191.
[6]Richardson S D,Thruston A D,Caughran T V,et al.Identification of new ozone disinfection byproducts in drinking water[J].Environmental Science&Technology,1999,33(19):3368-3377.
[7]高乃云,楚文海,徐斌.从生成机制谈饮用水中新型消毒副产物的控制策略[J].给水排水,2017,43(2):1-5.
[8]Chu W H,Gao N Y,Yin D Q,et al.Trace determination of 13haloacetamides in drinking water using liquid chromatography triple quadrupole mass spectrometry with atmospheric pressure chemical ionization[J].Journal of Chromatography A,2012,1235:178-181.
[9]Plewa M J,Muellner M G,Richardson S D,et al.Occurrence,synthesis,and mammalian cell cytotoxicity and genotoxicity of haloacetamides:an emerging class of nitrogenous drinking water disinfection byproducts[J].Environmental Science&Technology,2008,42(3):955-961.
[10]赵玉丽,李杏放.饮用水消毒副产物:化学特征与毒性[J].环境化学,2011,30(1):20-33.Zhao Y L,Li X F.Drinking water disinfection byproducts:chemical characterization and toxicity[J].Environmental Chemistry,2011,30(1):20-33.
[11]Krasner S W,Weinberg H S,Richardson S D,et al.Occurrence of a new generation of disinfection byproducts[J].Environmental Science&Technology,2006,40(23):7175-7185.
[12]Liew D,Linge K L,Joll C A,et al.Determination of halonitromethanes and haloacetamides:an evaluation of sample preservation and analyte stability in drinking water[J].Journal of Chromatography A,2012,1241:117-122.
[13]Kosaka K,Ohkubo K,Akiba M.Occurrence and formation of haloacetamides from chlorination at water purification plants across Japan[J].Water Research,2016,106:470-476.
[14]Zhang Y,Zhang Z Y,Zhao Y P,et al.Identifying health effects of exposure to trichloroacetamide using transcriptomics and metabonomics in mice(Mus musculus)[J].Environmental Science&Technology,2013,47(6):2918-2924.
[15]杨世迎,张宜涛,郑迪.高级还原技术:一种水处理新技术[J].化学进展,2016,28(6):934-941.Yang S Y,Zhang Y T,Zheng D.Advanced reduction processes:a novel technology for water treatment[J].Progress in Chemistry,2016,28(6):934-941.
[16]Yu H,Nie E,Xu J,et al.Degradation of diclofenac by advanced oxidation and reduction processes:kinetic studies,degradation pathways and toxicity assessments[J].Water Research,2013,47(5):1909-1918.
[17]Li X C,Ma J,Liu G F,et al.Efficient reductive dechlorination of monochloroacetic acid by sulfite/UV process[J].Environmental Science&Technology,2012,46(13):7342-7349.
[18]Liu X,Vellanki B P,Batchelor B,et al.Degradation of 1,2-dichloroethane with advanced reduction processes(ARPs):effects of process variables and mechanisms[J].Chemical Engineering Journal,2014,237:300-307.
[19]Kaushik V,Duan Y H,Jung B,et al.Arsenic removal using advanced reduction process with dithionite/UV-A kinetic study[J].Journal of Water Process Engineering,2018,23:314-319.
[20]Yazdanbakhsh A,Eslami A,Moussavi G,et al.Photo-assisted degradation of 2,4,6-trichlorophenol by an advanced reduction process based on sulfite anion radical:degradation,dechlorination and mineralization[J].Chemosphere,2018,191:156-165.
[21]Vellanki B P,Batchelor B,Abdel-Wahab A.Advanced reduction processes:a new class of treatment processes[J].Environmental Engineering Science,2013,30(5):264-271.
[22]韩慧丽,王宏杰,董文艺.真空紫外-亚硫酸盐法降解PFOS影响因素[J].环境科学,2017,38(4):1477-1482.Han H L,Wang H J,Dong W Y.Influencing factors on the degradation of PFOS through VUV-SO2-3[J].Environmental Science,2017,38(4):1477-1482.
[23]Chu W H,Ding S K,Bond T,et al.Zero valent iron produces dichloroacetamide from chloramphenicol antibiotics in the absence of chlorine and chloramines[J].Water Research,2016,104:254-261.
[24]Gu Y,Dong W,Luo C,et al.Efficient reductive decomposition of perfluorooctanesulfonate in a high photon flux UV/sulfite system[J].Environmental Science&Technology,2016,50(19):10554-10561.
[25]Li X C,Fang J Y,Liu G F,et al.Kinetics and efficiency of the hydrated electron-induced dehalogenation by the sulfite/UVprocess[J].Water Research,2014,62:220-228.
[26]Xiao Q,Ren Y F,Yu S L.Pilot study on bromate reduction from drinking water by UV/sulfite systems:economic cost comparisons,effects of environmental parameters and mechanisms[J].Chemical Engineering Journal,2017,330:1203-1210.
[27]Liu X,Yoon S,Batchelor B,et al.Degradation of vinyl chloride(VC)by the sulfite/UV advanced reduction process(ARP):effects of process variables and a kinetic model[J].Science of the Total Environment,2013,454-455:578-583.
[28]Liu X W,Zhang T Q,Shao Y.Aqueous bromate reduction by UV activation of sulfite[J].CLEAN-Soil,Air,Water,2014,42(10):1370-1375.
[29]Xie B H,Li X C,Huang X F,et al.Enhanced debromination of4-bromophenol by the UV/sulfite process:Efficiency and mechanism[J].Journal of Environmental Sciences,2017,54:231-238.
[30]Song Z,Tang H Q,Wang N,et al.Reductive defluorination of perfluorooctanoic acid by hydrated electrons in a sulfite-mediated UV photochemical system[J].Journal of Hazardous Materials,2013,262:332-338.
[31]Liu X,Yoon S,Batchelor B,et al.Photochemical degradation of vinyl chloride with an advanced reduction process(ARP)-effects of reagents and pH[J].Chemical Engineering Journal,2013,215-216:868-875.
[32]Vellanki B P,Batchelor B.Perchlorate reduction by the sulfite/ultraviolet light advanced reduction process[J].Journal of Hazardous Materials,2013,262:348-356.
[33]Chu W H,Gao N Y,Deng Y.Stability of newfound nitrogenous disinfection by-products haloacetamides in drinking water[J].Chinese Journal of Organic Chemistry,2009,29(10):1569-1574.
[34]Ding S K,Wang F F,Chu W H,et al.Rapid degradation of brominated and iodinated haloacetamides with sulfite in drinking water:degradation kinetics and mechanisms[J].Water Research,2018,143:325-333.