受体模型在湖泊沉积物中PAHs、PFASs和OCPs源解析比较
|
摘要
受体模型是一类主要用于空气污染溯源的源解析方法,在沉积物中的应用研究较少。正定矩阵因子分析模型(positive matrix factorization,PMF)、Unmix模型和主成分分析-多元线性回归模型(principal component analysis-multiple linear regression,PCA-MLR)是3种应用较成熟的大气源解析模型。以江苏省、安徽省的湖泊沉积物为研究对象,分别使用3种模型对采集沉积物样品中不同种类的半挥发性有机污染物多环芳烃(polycyclic aromatic hydrocarbons,PAHs)、全氟化合物(perfluoroalkyl substances,PFASs)、有机氯农药(organochlorine pesticides,OCPs)进行源解析,并通过对比3种模型结果的来源、贡献和拟合效果,探索模型在沉积物中污染物源解析中的应用。结果表明:不同模型对3类污染物的溯源均呈现出一致的解析结果,并且不同模型计算所得的模拟值与实测值拟合结果良好,在沉积物中污染物源解析得到较好应用。源解析结果表明:研究区沉积物中PAHs的来源主要有3种,分别为交通排放源,煤炭燃烧,天然气、柴油燃烧源;PFASs来源主要有3种,分别是氟化物加工助剂、树脂涂层、金属电镀工业源,纺织、贵金属、涂料工业排放源,纸质食品包装工业源;OCPs来源主要是滴滴涕和六氯环己烷(hexachlorocyclohexane,BHC)的历史残留,以及少量的异狄氏剂醛、氯丹和硫丹的贡献。PMF模型可以根据输入数据的不确定性赋予数据相应的权重。Unmix模型可以筛选出源信息较为明确的物质进入模型中。PCA-MLR模型可以定量的说明聚类分析的结果。应用多种模型进行污染物源解析可以使模型优缺点互补,消除单一模型局限性,更准确地完成沉积物中的污染物源解析。
Receptor models were typically used in air pollution studies and few publications are available for receptor models that consider the details of parameters and procedures in evaluating the trace organic pollutants in sediments. PMF, Unmix and PCA-MLR are three receptor modes which have been widely used in source apportionment analysis in air pollution study. The sediment samples were collected from seven lakes in Jiangsu and Anhui provinces. Three models were applied to analyze the source apportionment of different semi volatile organic pollutants, polycyclic aromatic hydrocarbons( PAHs), perfluoroalkyl substances( PFASs) and organochlorinepesticides( OCPs). The aims of this study were to explore the applications of the three receptor models in the sediment pollution, based on a comparison of their modeling results. The three models exhibit consistent results,and the simulated values and measured values fit well, indicating that these models are well applied in the source apportionment of sediment pollutants. The results show that PAHs in the sediment in the study area are mainly from three sources, including vehicle exhaust, coal combustion and kerosene combustion. There are three main sources of PFASs in the sediment, including fluoropolymer processing aid, fluororesin coating and metal plating, textile treatments, precious metals and coatings industry, and food paper packing. The source of OCPs is mainly pesticide residues, including DDTs, hexachlorocyclohexane( BHC), and some endrin aldehyde, chlordane and sulfudan.Among the three receptor models, PMF can give corresponding weight to the data based on the uncertainty of the input data, Unmix has advantage of selecting indicators associated to specific sources into the model, while PCAMLR can quantify the results of cluster analysis. Using multiple models to analyze the source apportionment of sediment pollutant can make the models complementary and the results more accurate, avoiding the limitation of a single model.
Receptor models were typically used in air pollution studies and few publications are available for receptor models that consider the details of parameters and procedures in evaluating the trace organic pollutants in sediments. PMF, Unmix and PCA-MLR are three receptor modes which have been widely used in source apportionment analysis in air pollution study. The sediment samples were collected from seven lakes in Jiangsu and Anhui provinces. Three models were applied to analyze the source apportionment of different semi volatile organic pollutants, polycyclic aromatic hydrocarbons( PAHs), perfluoroalkyl substances( PFASs) and organochlorinepesticides( OCPs). The aims of this study were to explore the applications of the three receptor models in the sediment pollution, based on a comparison of their modeling results. The three models exhibit consistent results,and the simulated values and measured values fit well, indicating that these models are well applied in the source apportionment of sediment pollutants. The results show that PAHs in the sediment in the study area are mainly from three sources, including vehicle exhaust, coal combustion and kerosene combustion. There are three main sources of PFASs in the sediment, including fluoropolymer processing aid, fluororesin coating and metal plating, textile treatments, precious metals and coatings industry, and food paper packing. The source of OCPs is mainly pesticide residues, including DDTs, hexachlorocyclohexane( BHC), and some endrin aldehyde, chlordane and sulfudan.Among the three receptor models, PMF can give corresponding weight to the data based on the uncertainty of the input data, Unmix has advantage of selecting indicators associated to specific sources into the model, while PCAMLR can quantify the results of cluster analysis. Using multiple models to analyze the source apportionment of sediment pollutant can make the models complementary and the results more accurate, avoiding the limitation of a single model.
引文
[1]陈锋.松花江流域水环境中多环芳烃的源解析方法与应用研究[D].北京:中国地质大学(北京),2016.CHEN F.Study on the methods of source apportionment of polycyclic aromatic hydrocarbons and the application in Songhua River[D].Beijing:China University of Geosciences(Beijing),2016.
[2]胡成,王彤,苏丹,等.水环境中污染物的源解析方法及其应用[J].水资源保护,2010,26(1):57-62.HU C,WANG T,SU D,et al.Methods for source apportionment of contaminates and their application in aquatic environment[J].Water Resources Protection,2010,26(1):57-62.
[3]KARAKAS F,IMAMOGLU I,GEDIK K.Positive matrix factorization dynamics in fingerprinting:a comparative study of PMF2 and EPA-PMF3 for source apportionment of sediment polychlorinated biphenyls[J].Environmental Pollution,2017,220:20-28.
[4]CONTINI D,CESARI D,CONTE M,et al.Application of PMF and CMB receptor models for the evaluation of the contribution of a large coal-fired power plant to PM10concentrations[J].Science of Total Environment,2016,560/561:131-140.
[5]STOJICA,STANISICS,MIJICZ,et al.Spatio-temporal distribution of VOC emissions in urban area based on receptor modeling[J].Atmospheric Environment,2015,106:71-79.
[6]PERRONE M G,LARSEN B R,FERRERO L,et al.Sources of high PM2.5concentrations in Milan,Northern Italy:molecular marker data and CMB modelling[J].Science of the Total Environment,2012,414:343-55.
[7]CHEN H Y,TENG Y G,WANG J S.Source apportionment of polycyclic aromatic hydrocarbons(PAHs)in surface sediments of the Rizhao coastal area(China)using diagnostic ratios and factor analysis with nonnegative constraints[J].Science of the Total Environment,2012,414:293-300.
[8]LI G,LANG Y,GAO M,et al.Carcinogenic and mutagenic potencies for different PAHs sources in coastal sediments of Shandong peninsula[J].Marine Pollution Bulletin,2014,84(1):418-423.
[9]FENG J,LIU M,LIU S,et al.Source apportionment and risk assessment of polycyclic aromatic hydrocarbons(PAHs)in surface sediments from upper reach of Huaihe River,China[J].Polycyclic Aromatic Compounds,2015,35(5):416-427.
[10]HO C C,CHAN C C,CHIO C P,et al.Source apportionment of mass concentration and inhalation risk with long-term ambient PCDD/Fs measurements in an urban area[J].Journal of Hazardous Materials,2016,317:180-187.
[11]ZHANG Y,GUO F,MENG W,et al.Water quality assessment and source identification of Daliao River basin using multivariate statistical methods[J].Environmental Monitoring and Assessment,2009,152(1/2/3/4):105-121.
[12]林秀梅,陈江麟,刘文新,等.多元统计在渤海表层沉积物中PAHs源解析上的应用[J].海洋环境科学,2007(2):107-111.LIN X M,CHEN J L,LIU W X,et al.Source identification of PAHs in surface sediments from Bohai Sea by multivariate statistics[J].Marine Environmental Science,2007(2):107-111.
[13]YAN Y,HE Q,GUO L,et al.Source apportionment and toxicity of atmospheric polycyclic aromatic hydrocarbons by PMF:quantifying the influence of coal usage in Taiyuan,China[J].Atmospheric Research,2017,193:50-59.
[14]GARY N,RACHELLE D.EPA PMF 5.0 user guide[M].Washington DC:US EPA,2014.
[15]HENRY R C.Duality in multivariate receptor models[J].Chemometrics and Intelligent Laboratory Systems,2005,77(1/2):59-63.
[16]QI Y,HUO S,XI B,et al.Spatial distribution and source apportionment of PFASs in surface sediments from five lake regions,China[J].Scientific Reports,2016,6:22674.
[17]LI C,HUO S,YU Z,et al.National investigation of semi-volatile organic compounds(PAHs,OCPs,and PCBs)in lake sediments of China:occurrence,spatial variation and risk assessment[J].Science of Total Environment,2017,579:325-336.
[18]PREVEDOUROS K,COUSINS I T,BUCK R C,et al.Sources,fate and transport of perfluorocarboxylates[J].Environmental Science and Technology,2006,40(1):32-44.
[19]LI L,ZHAI Z H,LIU J G,et al.Estimating industrial and domestic environmental releases of perfluorooctanoic acid and its salts in China from 2004 to 2012[J].Chemosphere,2015,129:100-109.
[20]MARTINEZ-MORAL M P,TENA M T.Determination of perfluorocompounds in popcorn packaging by pressurised liquid extraction and ultra-performance liquid chromatography-tandem mass spectrometry[J].Talanta,2012,101:104-109.
[21]XIE S W,LU Y L,WANG T Y,et al.Estimation of PFOS emission from domestic sources in the eastern coastal region of China[J].Environment International,2013,59:336-343.
[22]YANG B,ZHOU L L,XUE N D,et al.Source apportionment of polycyclic aromatic hydrocarbons in soils of Huanghuai Plain,China:comparison of three receptor models[J].Science of Total Environment,2013,443:31-39.
[23]WANG Z,CHEN J,YANG P,et al.Polycyclic aromatic hydrocarbons in Dalian soils:distribution and toxicity assessment[J].Journal of Environmental Monitoring,2007,9(2):199-204.
[24]MOSTERT M M R,AYOKO G A,KOKOT S.Application of chemometrics to analysis of soil pollutants[J].Trac Trends in Analytical Chemistry,2010,29(5):430-445.
[25]LARSEN R K,BAKER J E.Source apportionment of polycyclic aromatic hydrocarbons in the urban atmosphere:a comparison of three methods[J].Environmental Science and Technology,2003,37:1873-1881.
[26]LIU Y,CHEN L,HUANG Q,et al.Source apportionment of polycyclic aromatic hydrocarbons(PAHs)in surface sediments of the Huangpu River,Shanghai,China[J].Science of Total Environment,2009,407(8):2931-2938.
[27]HU Y,QI S,ZHANG J,et al.Assessment of organochlorine pesticides contamination in underground rivers in Chongqing,Southwest China[J].Journal of Geochemical Exploration,2011,111(1):47-55.
[28]CALLEN M S,de la CRUZ M T,LOPEZ J M,et al.Comparison of receptor models for source apportionment of the PM10in Zaragoza(Spain)[J].Chemosphere,2009,76(8):1120-1129.
[2]胡成,王彤,苏丹,等.水环境中污染物的源解析方法及其应用[J].水资源保护,2010,26(1):57-62.HU C,WANG T,SU D,et al.Methods for source apportionment of contaminates and their application in aquatic environment[J].Water Resources Protection,2010,26(1):57-62.
[3]KARAKAS F,IMAMOGLU I,GEDIK K.Positive matrix factorization dynamics in fingerprinting:a comparative study of PMF2 and EPA-PMF3 for source apportionment of sediment polychlorinated biphenyls[J].Environmental Pollution,2017,220:20-28.
[4]CONTINI D,CESARI D,CONTE M,et al.Application of PMF and CMB receptor models for the evaluation of the contribution of a large coal-fired power plant to PM10concentrations[J].Science of Total Environment,2016,560/561:131-140.
[5]STOJICA,STANISICS,MIJICZ,et al.Spatio-temporal distribution of VOC emissions in urban area based on receptor modeling[J].Atmospheric Environment,2015,106:71-79.
[6]PERRONE M G,LARSEN B R,FERRERO L,et al.Sources of high PM2.5concentrations in Milan,Northern Italy:molecular marker data and CMB modelling[J].Science of the Total Environment,2012,414:343-55.
[7]CHEN H Y,TENG Y G,WANG J S.Source apportionment of polycyclic aromatic hydrocarbons(PAHs)in surface sediments of the Rizhao coastal area(China)using diagnostic ratios and factor analysis with nonnegative constraints[J].Science of the Total Environment,2012,414:293-300.
[8]LI G,LANG Y,GAO M,et al.Carcinogenic and mutagenic potencies for different PAHs sources in coastal sediments of Shandong peninsula[J].Marine Pollution Bulletin,2014,84(1):418-423.
[9]FENG J,LIU M,LIU S,et al.Source apportionment and risk assessment of polycyclic aromatic hydrocarbons(PAHs)in surface sediments from upper reach of Huaihe River,China[J].Polycyclic Aromatic Compounds,2015,35(5):416-427.
[10]HO C C,CHAN C C,CHIO C P,et al.Source apportionment of mass concentration and inhalation risk with long-term ambient PCDD/Fs measurements in an urban area[J].Journal of Hazardous Materials,2016,317:180-187.
[11]ZHANG Y,GUO F,MENG W,et al.Water quality assessment and source identification of Daliao River basin using multivariate statistical methods[J].Environmental Monitoring and Assessment,2009,152(1/2/3/4):105-121.
[12]林秀梅,陈江麟,刘文新,等.多元统计在渤海表层沉积物中PAHs源解析上的应用[J].海洋环境科学,2007(2):107-111.LIN X M,CHEN J L,LIU W X,et al.Source identification of PAHs in surface sediments from Bohai Sea by multivariate statistics[J].Marine Environmental Science,2007(2):107-111.
[13]YAN Y,HE Q,GUO L,et al.Source apportionment and toxicity of atmospheric polycyclic aromatic hydrocarbons by PMF:quantifying the influence of coal usage in Taiyuan,China[J].Atmospheric Research,2017,193:50-59.
[14]GARY N,RACHELLE D.EPA PMF 5.0 user guide[M].Washington DC:US EPA,2014.
[15]HENRY R C.Duality in multivariate receptor models[J].Chemometrics and Intelligent Laboratory Systems,2005,77(1/2):59-63.
[16]QI Y,HUO S,XI B,et al.Spatial distribution and source apportionment of PFASs in surface sediments from five lake regions,China[J].Scientific Reports,2016,6:22674.
[17]LI C,HUO S,YU Z,et al.National investigation of semi-volatile organic compounds(PAHs,OCPs,and PCBs)in lake sediments of China:occurrence,spatial variation and risk assessment[J].Science of Total Environment,2017,579:325-336.
[18]PREVEDOUROS K,COUSINS I T,BUCK R C,et al.Sources,fate and transport of perfluorocarboxylates[J].Environmental Science and Technology,2006,40(1):32-44.
[19]LI L,ZHAI Z H,LIU J G,et al.Estimating industrial and domestic environmental releases of perfluorooctanoic acid and its salts in China from 2004 to 2012[J].Chemosphere,2015,129:100-109.
[20]MARTINEZ-MORAL M P,TENA M T.Determination of perfluorocompounds in popcorn packaging by pressurised liquid extraction and ultra-performance liquid chromatography-tandem mass spectrometry[J].Talanta,2012,101:104-109.
[21]XIE S W,LU Y L,WANG T Y,et al.Estimation of PFOS emission from domestic sources in the eastern coastal region of China[J].Environment International,2013,59:336-343.
[22]YANG B,ZHOU L L,XUE N D,et al.Source apportionment of polycyclic aromatic hydrocarbons in soils of Huanghuai Plain,China:comparison of three receptor models[J].Science of Total Environment,2013,443:31-39.
[23]WANG Z,CHEN J,YANG P,et al.Polycyclic aromatic hydrocarbons in Dalian soils:distribution and toxicity assessment[J].Journal of Environmental Monitoring,2007,9(2):199-204.
[24]MOSTERT M M R,AYOKO G A,KOKOT S.Application of chemometrics to analysis of soil pollutants[J].Trac Trends in Analytical Chemistry,2010,29(5):430-445.
[25]LARSEN R K,BAKER J E.Source apportionment of polycyclic aromatic hydrocarbons in the urban atmosphere:a comparison of three methods[J].Environmental Science and Technology,2003,37:1873-1881.
[26]LIU Y,CHEN L,HUANG Q,et al.Source apportionment of polycyclic aromatic hydrocarbons(PAHs)in surface sediments of the Huangpu River,Shanghai,China[J].Science of Total Environment,2009,407(8):2931-2938.
[27]HU Y,QI S,ZHANG J,et al.Assessment of organochlorine pesticides contamination in underground rivers in Chongqing,Southwest China[J].Journal of Geochemical Exploration,2011,111(1):47-55.
[28]CALLEN M S,de la CRUZ M T,LOPEZ J M,et al.Comparison of receptor models for source apportionment of the PM10in Zaragoza(Spain)[J].Chemosphere,2009,76(8):1120-1129.