阿哈水库DOM的分离及其对消毒副产物的贡献
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摘要
为研究高原喀斯特湖库DOM(dissolved organic matter,溶解性有机质)的组成及其化学特征对DBPs(disinfection byproducts,消毒副产物)生成路径的影响,以西南喀斯特地区贵阳市阿哈水库的DOM为研究对象,结合XAD大孔树脂分离技术,通过化学表征[包括UV-Vis(紫外-可见光光谱)、FTIR(红外光谱)和3D-EEM(三维荧光光谱)]手段来研究各组分对C-DBPs(含碳消毒副产物)和N-DBPs(含氮消毒副产物)的生成贡献.不同组分芳香性的大小依次为HON(憎水中性物)>HIB(亲水碱)>HOA(憎水酸)>HIN(亲水中性物)≈HIA(亲水酸)>HOB(憎水碱).憎水与亲水DOM的DBPs生成潜能相近.其中,HON最高,其次为HIB和HOA.HIB和HOA的主要卤代反应位分别来源于藻类有机物的蛋白质和富里酸,而HON的DBPs生成潜能的贡献主要为分子中的芳香和共轭不饱和结构.HIA和HIN的构成主要为脂肪烃,贡献较低的DBPs的生成潜能.对于C-DBPs,THMs和HAAs的生成潜能总体相近,不同组分的差异明显.对于N-DBPs,卤乙腈的生成潜能占80%以上,憎水DOM的贡献较高.DBPs的生成路径从UV-Vis、FTIR和3D-EEM的官能团和特征峰解析结果中均得到了较好的响应.
This paper investigates the relationship between disinfection by-products(DBPs) formation pathways and components with various chemical characteristics of dissolved organic matter(DOM) in a Karst plateau reservoir,Aha Reservoir in Guiyang City. Using DOM obtained from the reservoir,several chemical characterization approaches,including UV-Vis scanning,FTIR,and 3 D-EEM fluoresce,were applied to investigate the potential contribution of different DOM fractions(separated by XAD resin) in the generation of the carbonaceous and nitrogenous DBPs(C-DBPs and N-DBPs). The results indicated that the aromaticity of different DOM fractions followed in the decreasing order: hydrophobic neutral(HON) > hydrophilic base(HIB) > hydrophobic acid(HOA) > hydrophilic neutral(HIN) ≈hydrophilic acid(HIA) >hydrophobic base(HOB). Both hydrophilic and hydrophobic fractions possessed similar DBP formation potentials(DBPFPs). In detail,HON had the highest DBPFP,followed by HIB and HOA. The majority of halogenated active sites in HIB and HOA originated from protein in algal organic matter and fulvic acid,while the DBPFP of HON is likely responsible for its high aromatic and unsaturated structures. The decreasing DBPFP corresponded with elevated aliphatic hydrocarbon structures found in HIN and HIA. For C-DBPs,less difference was observed for THMs and HAAs of all DOM fractions. Haloacetonitriles accounted for 80% of N-DBPs,which was mainly contributed by hydrophobic parts. The DBP formation pathway was satisfactorily supported from chemicalfunctional groups and characteristic peaks by UV-Vis,FTIR,and 3 D-EEM,respectively.
This paper investigates the relationship between disinfection by-products(DBPs) formation pathways and components with various chemical characteristics of dissolved organic matter(DOM) in a Karst plateau reservoir,Aha Reservoir in Guiyang City. Using DOM obtained from the reservoir,several chemical characterization approaches,including UV-Vis scanning,FTIR,and 3 D-EEM fluoresce,were applied to investigate the potential contribution of different DOM fractions(separated by XAD resin) in the generation of the carbonaceous and nitrogenous DBPs(C-DBPs and N-DBPs). The results indicated that the aromaticity of different DOM fractions followed in the decreasing order: hydrophobic neutral(HON) > hydrophilic base(HIB) > hydrophobic acid(HOA) > hydrophilic neutral(HIN) ≈hydrophilic acid(HIA) >hydrophobic base(HOB). Both hydrophilic and hydrophobic fractions possessed similar DBP formation potentials(DBPFPs). In detail,HON had the highest DBPFP,followed by HIB and HOA. The majority of halogenated active sites in HIB and HOA originated from protein in algal organic matter and fulvic acid,while the DBPFP of HON is likely responsible for its high aromatic and unsaturated structures. The decreasing DBPFP corresponded with elevated aliphatic hydrocarbon structures found in HIN and HIA. For C-DBPs,less difference was observed for THMs and HAAs of all DOM fractions. Haloacetonitriles accounted for 80% of N-DBPs,which was mainly contributed by hydrophobic parts. The DBP formation pathway was satisfactorily supported from chemicalfunctional groups and characteristic peaks by UV-Vis,FTIR,and 3 D-EEM,respectively.
引文
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[17]李磊,李秋华,焦树林,等.阿哈水库浮游植物功能群时空分布特征及其影响因子分析[J].环境科学学报,2015,35(11):3604-3611.LI Lei,LI Qiuhua,JIAO Shulin,et al.Spatial and temporal distribution characteristics of phytoplankton functional groups in Aha Reservoir and their influencing factors[J].Acta Scientiae Circumstantiae,2015,35(11):3604-3611.
[18]姚新建,文金淼.天然有机物的提取与分离[J].化工技术与开发,2011,40(10):25-28.YAO Xinjian,WEN Jinmiao.Extraction and separation of natural organic matter[J].Technology&Development of Chemical Industry,2011,40(10):25-28.
[19]WANG Zhikang,KIM J,SEO Y.Influence of bacterial extracellular polymeric substances on the formation of carbonaceous and nitrogenous disinfection byproducts[J].Environmental Science&Technology,2012,46(20):11361-11369.
[20]CHEN Wen,WESTERHOFF P,LEENHEER J A,et al.Fluorescence excitation-emission matrix regional integration to quantify spectra for dissolved organic matter[J].Environmental Science&Technology,2003,37(24):5701-5710.
[21]NEBBIOSO A,PICCOLO A.Molecular characterization of dissolved organic matter(DOM):a critical review[J].Analytical and Bioanalytical Chemistry,2013,405(1):109-124.
[22]谢理,杨浩,渠晓霞,等.滇池典型陆生和水生植物溶解性有机质组分的光谱分析[J].环境科学研究,2013,26(1):72-79.XIE Li,YANG Hao,QU Xiaoxia,et al.Characterization of water extractable organic matters from the dominant plants in Lake Dianchi by multiple spectroscopic techniques[J].Research of Environmental Sciences,2013,26(1):72-79.
[23]MATILAINEN A,VEPSALAINEN M,SILLANPAA M.Natural organic matter removal by coagulation during drinking water treatment:a review[J].Advances in Colloid and Interface Science,2010,159(2):189-197.
[24]焦中志,陈忠林,李作良,等.南方某水源水中天然有机物的特点及氯胺对氯化消毒副产物的控制[J].环境工程学报,2007,1(12):79-82.JIAO Zhongzhi,CHEN Zhonglin,LI Zuoliang,et al.Characters of natural organic mattters in south water resource and the control of DBPs by chloramine compared with chlorine[J].Chinese Journal of Environmental Engineering,2007,1(12):79-82.
[25]KANOKKANTAPONG V,MARHABA T F,PANYAPINYOPHOL B,et al.FTIR evaluation of functional groups involved in the formation of haloacetic acids during the chlorination of raw water[J].Journal of Hazardous Materials,2006,136(2):188-196.
[26]KANOKKANTAPONG V,MARHABA T F,PAVASANT P,et al.Characterization of haloacetic acid precursors in source water[J].Journal of Environmental Management,2006,80(3):214-221.
[27]BOND T,HUANG J,TEMPLETON M R,et al.Occurrence and control of nitrogenous disinfection by-products in drinking water-a review[J].Water Research,2011,45(15):4341-4354.
[28]BOND T,TEMPLETON M R,GRAHAM N.Precursors of nitrogenous disinfection by-products in drinking water-a critical review and analysis[J].Journal of Hazardous Materials,2012,235/236(2):1-16.
[29]TANG Xiaomin,ZHENG Huaili,GAO Baoyu,et al.Interactions of specific extracellular organic matter and polyaluminum chloride and their roles in the algae-polluted water treatment[J].Journal of Hazardous Materials,2017,332:1-9.
[30]ZHOU Shiqing,SHAO Yisheng,GAO Naiyun,et al.Removal of Microcystis aeruginosa by potassium ferrate(VI):impacts on cells integrity,intracellular organic matter release and disinfection byproducts formation[J].Chemical Engineering Journal,2014,251(5):304-309.
[31]NIKOLAOU A D,LEKKAS T D.The role of natural organic matter during formation of chlorination by-products:a review[J].Acta Hydrochimica et Hydrobiologica,2001,29(2/3):63-77.
[32]WANG Zhikang,CHOI O,SEO Y.Relative contribution of biomolecules in bacterial extracellular polymeric substances to disinfection byproduct formation[J].Environmental Science&Technology,2013,47(17):9764-9773.
[33]CHEN Jie,GU Baohua,LEBOEUF E J,et al.Spectroscopic characterization of the structural and functional properties of natural organic matter fractions[J].Chemosphere,2002,48(1):59-68.
[34]CHANG Huihsien,CHEN Chiayang,WANG Genshuh.Characteristics of C-,N-DBPs formation from nitrogen-enriched dissolved organic matter in raw water and treated wastewater effluent[J].Water Research,2013,47(8):2729-2741.
[35]RICHARDSON S D,POSTIGO C.Drinking water disinfection byproducts,emerging organic contaminants and human health[M].Barcelona Spain:Springer Berlin Heidelberg,2012:93-137.
[2]方晶云.蓝藻细胞及藻类有机物在氯化消毒中副产物的形成机理与控制[D].哈尔滨:哈尔滨工业大学,2010.
[3]张冉.饮用水源中天然有机物特性表征及有机物强化去除工艺研究[D].石家庄:河北科技大学,2009.
[4]WANG Zhikang,HESSLER C M,XUE Zheng,et al.The role of extracellular polymeric substances on the sorption of natural organic matter[J].Water Research,2012,46(4):1052-1060.
[5]RICHARDSON S D,PLEWA M J,WAGNER E D,et al.Occurrence,genotoxicity,and carcinogenicity of regulated and emerging disinfection by-products in drinking water:a review and roadmap for research[J].Mutation Research/Reviews in Mutation Research,2007,636(1/2/3):178-242.
[6]刘艳芳,王启山,鲁金凤,等.原水天然有机物化学特性与消毒副产物关系[J].水处理技术,2010,36(2):25-28.LIU Yanfang,WANG Qishan,LU Jinfeng,et al.Chemical characteristics of natural organic matter and its relationship with disinfection by-product in drinking water[J].Technology of Water Treatment,2010,36(2):25-28.
[7]王立英,吴丰昌,张润宇,等.红枫湖溶解有机质不同有机组分的地球化学特征[C]//中国矿物岩石地球化学学会,中国科学院地球化学研究所.贵阳:中国矿物岩石地球化学学会第12届学术年会论文集,2009:413.
[8]王立英,吴丰昌,张润宇.应用XAD系列树脂分离和富集天然水体中溶解有机质的研究进展[J].地球与环境,2006,34(1):90-96.WANG Liying,WU Fengchang,ZHANG Runyu.A method of separate and concentrate dissolved organic matter by XAD resin in natural aquatic systems[J],Earth and Environment,2006,34(1):90-96.
[9]郭瑾,马军.松花江水中天然有机物的提取分离与特性表征[J].环境科学,2005,26(5):77-84.GUO Jin,MA Jun.Characterization of isolated fractions of NOM from Songhua River[J].Environmental Science,2005,26(5):77-84.
[10]王立英,张润宇,吴丰昌.贵州红枫湖溶解有机质不同分离组分的卤代活性研究[J].农业环境科学学报,2012,31(10):2006-2012.WANG Liying,ZHANG Runyu,WU Fengchang.Chlorination activity of dissolved organic matter fractions in Hongfeng Lake,Guizhou,China[J].Journal of Agro-Environment Science,2012,31(10):2006-2012.
[11]王志康,李玥,桂昕,等.贵阳市红枫湖天然有机物化学特征初步调查[J].环保科技,2017,23(2):1-4.WANG Zhikang,LI Yue,GUI Xin,et al.Primiary investigation on chemical characteristics of natural organic matter in Hongfeng Lake,Guiyang[J].Journal of Environmental Techonology,2017,23(2):1-4.
[12]岳兰秀,吴丰昌,陈文龙.贵州百花湖水中溶解有机质的分子量分布随深度的变化规律[J].环境科学与管理,2008,33(5):66-70.YUE Lanxiu,WU Fengchang,CHEN Wenlong.Changes in molecular weight distribution of dissolved organic matter with depth in Lake Baihua[J].Environmental Science and Management,2008,33(5):66-70.
[13]方志青,李存雄,张明时,等.百花湖、阿哈水库底泥及营养盐蓄积量的估算[J].贵州师范大学学报(自然科学版),2009,27(4):30-33.FANG Zhiqing,LI Cunxiong,ZHANG Mingshi,et al.Sediment deposition and its nutrient volume in Baihua Lake and Aha Lake[J].Journal of Guizhou Normal University(Natural Sciences),2009,27(4):30-33.
[14]刘鸿雁,王龙飞,罗梅,等.贵阳市阿哈水库农业面源污染调查与分析[J].贵州农业科学,2009,37(9):235-239.LIU Hongyan,WANG Longfei,LUO Mei,et al.Investigation and analysis on widespread pollution from the overuse of fertilizer and pesticides around Aha Reservior in Guiyang City[J].Guizhou Agricultural Sciences,2009,37(9):235-239.
[15]潘祖光,侯克钧.关于阿哈水库水质及污染情况的研究及对策[J].贵州工业大学学报(自然科学版),2007,36(4):60-63.PAN Zuguang,HOU Kejun.Research and strategies on the water quality and pollution situation in the Aha Lake[J].Journal of Guizhou University of Technology(Natural Science Edition),2007,36(4):60-63.
[16]陈作州.阿哈水库、红枫湖水库水华蓝藻的时空变化及毒性试验研究[D].贵阳:贵州师范大学,2007.
[17]李磊,李秋华,焦树林,等.阿哈水库浮游植物功能群时空分布特征及其影响因子分析[J].环境科学学报,2015,35(11):3604-3611.LI Lei,LI Qiuhua,JIAO Shulin,et al.Spatial and temporal distribution characteristics of phytoplankton functional groups in Aha Reservoir and their influencing factors[J].Acta Scientiae Circumstantiae,2015,35(11):3604-3611.
[18]姚新建,文金淼.天然有机物的提取与分离[J].化工技术与开发,2011,40(10):25-28.YAO Xinjian,WEN Jinmiao.Extraction and separation of natural organic matter[J].Technology&Development of Chemical Industry,2011,40(10):25-28.
[19]WANG Zhikang,KIM J,SEO Y.Influence of bacterial extracellular polymeric substances on the formation of carbonaceous and nitrogenous disinfection byproducts[J].Environmental Science&Technology,2012,46(20):11361-11369.
[20]CHEN Wen,WESTERHOFF P,LEENHEER J A,et al.Fluorescence excitation-emission matrix regional integration to quantify spectra for dissolved organic matter[J].Environmental Science&Technology,2003,37(24):5701-5710.
[21]NEBBIOSO A,PICCOLO A.Molecular characterization of dissolved organic matter(DOM):a critical review[J].Analytical and Bioanalytical Chemistry,2013,405(1):109-124.
[22]谢理,杨浩,渠晓霞,等.滇池典型陆生和水生植物溶解性有机质组分的光谱分析[J].环境科学研究,2013,26(1):72-79.XIE Li,YANG Hao,QU Xiaoxia,et al.Characterization of water extractable organic matters from the dominant plants in Lake Dianchi by multiple spectroscopic techniques[J].Research of Environmental Sciences,2013,26(1):72-79.
[23]MATILAINEN A,VEPSALAINEN M,SILLANPAA M.Natural organic matter removal by coagulation during drinking water treatment:a review[J].Advances in Colloid and Interface Science,2010,159(2):189-197.
[24]焦中志,陈忠林,李作良,等.南方某水源水中天然有机物的特点及氯胺对氯化消毒副产物的控制[J].环境工程学报,2007,1(12):79-82.JIAO Zhongzhi,CHEN Zhonglin,LI Zuoliang,et al.Characters of natural organic mattters in south water resource and the control of DBPs by chloramine compared with chlorine[J].Chinese Journal of Environmental Engineering,2007,1(12):79-82.
[25]KANOKKANTAPONG V,MARHABA T F,PANYAPINYOPHOL B,et al.FTIR evaluation of functional groups involved in the formation of haloacetic acids during the chlorination of raw water[J].Journal of Hazardous Materials,2006,136(2):188-196.
[26]KANOKKANTAPONG V,MARHABA T F,PAVASANT P,et al.Characterization of haloacetic acid precursors in source water[J].Journal of Environmental Management,2006,80(3):214-221.
[27]BOND T,HUANG J,TEMPLETON M R,et al.Occurrence and control of nitrogenous disinfection by-products in drinking water-a review[J].Water Research,2011,45(15):4341-4354.
[28]BOND T,TEMPLETON M R,GRAHAM N.Precursors of nitrogenous disinfection by-products in drinking water-a critical review and analysis[J].Journal of Hazardous Materials,2012,235/236(2):1-16.
[29]TANG Xiaomin,ZHENG Huaili,GAO Baoyu,et al.Interactions of specific extracellular organic matter and polyaluminum chloride and their roles in the algae-polluted water treatment[J].Journal of Hazardous Materials,2017,332:1-9.
[30]ZHOU Shiqing,SHAO Yisheng,GAO Naiyun,et al.Removal of Microcystis aeruginosa by potassium ferrate(VI):impacts on cells integrity,intracellular organic matter release and disinfection byproducts formation[J].Chemical Engineering Journal,2014,251(5):304-309.
[31]NIKOLAOU A D,LEKKAS T D.The role of natural organic matter during formation of chlorination by-products:a review[J].Acta Hydrochimica et Hydrobiologica,2001,29(2/3):63-77.
[32]WANG Zhikang,CHOI O,SEO Y.Relative contribution of biomolecules in bacterial extracellular polymeric substances to disinfection byproduct formation[J].Environmental Science&Technology,2013,47(17):9764-9773.
[33]CHEN Jie,GU Baohua,LEBOEUF E J,et al.Spectroscopic characterization of the structural and functional properties of natural organic matter fractions[J].Chemosphere,2002,48(1):59-68.
[34]CHANG Huihsien,CHEN Chiayang,WANG Genshuh.Characteristics of C-,N-DBPs formation from nitrogen-enriched dissolved organic matter in raw water and treated wastewater effluent[J].Water Research,2013,47(8):2729-2741.
[35]RICHARDSON S D,POSTIGO C.Drinking water disinfection byproducts,emerging organic contaminants and human health[M].Barcelona Spain:Springer Berlin Heidelberg,2012:93-137.