浙江省农田土壤多环芳烃污染及风险评价
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摘要
为探究浙江省农田土壤中16种优控多环芳烃(Polycyclic aromatic hydrocarbons, PAHs)含量、来源及生态和健康风险,用网格布点法采集了62个农田土壤样品并进行实验分析。结果表明,∑PAHs浓度范围为34.04～1 990.38 ng·g~(-1),污染物以高环类PAHs为主,研究区域内所有土样苯并[a]芘(BaP)浓度均未超过我国新颁布的《土壤环境质量农用地土壤污染风险管控标准(试行)》(GB 15618—2018)中的风险筛选值。采用比值法及主成分分析研究其环境来源,结果显示主要来自于交通污染、煤炭和薪柴燃烧。内梅罗综合污染指数法评价结果表明,研究区有87.10%的样点存在生态风险。毒性当量因子风险评价法分析结果显示,PAHs的毒性当量浓度范围为1.53～268.27 ng·g~(-1),7种致癌PAHs为污染主体,平均占比高达99.18%。暴露量估算结果显示,经口摄入是PAHs致癌风险最高的暴露途径。健康风险评价显示,土壤中PAHs暴露暂时不会对人群产生明显的非致癌风险,但儿童的综合致癌风险已超过可接受范围,需引起重视。
In this study, gridded field observations at 62 sites were undertaken to determine the concentration, composition, sources, and ecological and health risks of 16 polycyclic aromatic hydrocarbons(PAHs)in Zhejiang Province. The methods consisted of Soxhlet extraction and silica gel column chromatography, followed by gas chromatography–mass spectrometry(GC–MS). The concentrations of ΣPAHs ranged from 34.04 ng·g~(-1) to 1 990.38 ng·g~(-1), and high molecular weight PAHs were dominant in all soils. The level of benzo[a]pyrene(BaP)was lower than the National Soil Environmental Quality Standard(GB15618—2018). Source diagnostic ratio and principal component analysis showed that vehicle emissions, and coal and biomass combustion, were the main sources of PAHs. According to Nemerow′s pollution index, ecological risks extensively exist in 87.10% of the sampling sites. Toxic equivalents of PAHs ranged from 1.53 ng·g~(-1) to 268.27 ng·g~(-1), in which 7 carcinogenic PAHs contributed 99.18%. PAHs exposures of adults and children via ingestion, dermal absorption,and inhalation were estimated. I Ingestion was found to be the most important PAHs exposure pathway, and non-carcinogenic risks were negligible, while the comprehensive carcinogenic risk for children exceeded acceptable levels. This research provides useful information on human exposure to PAHs in farmland soils of Zhejiang Province, and is valuable for policy makers and scientists.
In this study, gridded field observations at 62 sites were undertaken to determine the concentration, composition, sources, and ecological and health risks of 16 polycyclic aromatic hydrocarbons(PAHs)in Zhejiang Province. The methods consisted of Soxhlet extraction and silica gel column chromatography, followed by gas chromatography–mass spectrometry(GC–MS). The concentrations of ΣPAHs ranged from 34.04 ng·g~(-1) to 1 990.38 ng·g~(-1), and high molecular weight PAHs were dominant in all soils. The level of benzo[a]pyrene(BaP)was lower than the National Soil Environmental Quality Standard(GB15618—2018). Source diagnostic ratio and principal component analysis showed that vehicle emissions, and coal and biomass combustion, were the main sources of PAHs. According to Nemerow′s pollution index, ecological risks extensively exist in 87.10% of the sampling sites. Toxic equivalents of PAHs ranged from 1.53 ng·g~(-1) to 268.27 ng·g~(-1), in which 7 carcinogenic PAHs contributed 99.18%. PAHs exposures of adults and children via ingestion, dermal absorption,and inhalation were estimated. I Ingestion was found to be the most important PAHs exposure pathway, and non-carcinogenic risks were negligible, while the comprehensive carcinogenic risk for children exceeded acceptable levels. This research provides useful information on human exposure to PAHs in farmland soils of Zhejiang Province, and is valuable for policy makers and scientists.
引文
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[26]Chen Y N,Zhang J Q,Zhang F,et al.Contamination and health risk assessment of PAHs in farmland soils of the Yinma River Basin,China[J].Ecotoxicology and Environmental Safety,2018,156:383-390.
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[29]Chung M K,Hu R,Cheung K C,et al.Pollutants in Hong Kong soils:Polycyclic aromatic hydrocarbons[J].Chemosphere,2007,67(3):464-387473.
[30]Marquez-Bravo L G,Briggs D,Shayler H,et al.Concentrations of polycyclic aromatic hydrocarbons in New York City community garden soils:Potential sources and influential factors[J].Environmental Toxicology&Chemistry,2016,35(2):357-367.
[31]VROM.Environmental quality objectives in the Netherlands:A review of environmental quality objectives and their policy framework in the Netherlands[M].The Hague:Ministry of Housing,Spatial Planning and the Environment,1994.
[32]Yunker M B,Macdonald R W,et al.PAHs in the Fraser River basin:A critical appraisal of PAH ratios as indicators of PAH source and composition[J].Organic Geochemistry,2002,33(4):489-515.
[33]Rocher V,Azimi S,Régis M,et al.Hydrocarbons and heavy metals in the different sewer deposits in the‘Le Marais’catchment(Paris,France):Stocks,distributions and origins[J].Science of the Total Environment,2004,323(1/2/3):107-122.
[34]Lee B K,Dong T T T.Toxicity and source assignment of polycyclic aromatic hydrocarbons in road dust from urban residential and industrial areas in a typical industrial city in Korea[J].Journal of Material Cycles and Waste Management,2011,13(1):34-42.
[35]周玲莉,薛南冬,李发生,等.黄淮平原农田土壤中多环芳烃的分布、风险及来源[J].中国环境科学,2012,32(7):1250-1256.ZHOU Ling-li,XUE Nan-dong,LI Fa-sheng,et al.Distribution,source analysis and risk assessment of polycyclic aromatic hydrocarbons in farmland soils in Huanghuai Plain[J].China Environmental Science,2012,32(7):1250-1256.
[36]吴焕波.区域大气环境污染源人体健康风险评价方法研究[D].兰州:兰州大学,2016.WU Huan-bo.Study on human health risk assessment method for regional atmospheric environmental pollution sources[D].Lanzhou:Lanzhou University,2016.
[2]Sun J H,Wang G L,Chai Y,et al.Distribution of polycyclic aromatic hydrocarbons(PAHs)in Henan Reach of the Yellow River,Middle China[J].Ecotoxicology and Environmental Safety,2009,72(5):1614-1624.
[3]Xu Y F,Dai S X,Meng K,et al.Occurrence and risk assessment of potentially toxic elements and typical organic pollutants in contaminated rural soils[J].Science of the Total Environment,2018,630:618-629.
[4]Jia J,Bi C,Guo X,et al.Characteristics,identification,and potential risk of polycyclic aromatic hydrocarbons in road dusts and agricultural soils from industrial sites in Shanghai,China[J].Environmental Science and Pollution Research,2017,24(1):605-615.
[5]Nemr A,El-Sadaawy M M,Khaled A,et al.Aliphatic and polycyclic aromatic hydrocarbons in the surface sediments of the Mediterranean:Assessment and source recognition of petroleum hydrocarbons[J].Environmental Monitoring and Assessment,2013,185(6):4571-4589.
[6]Lee Y N,Lee S,Kim J S,et al.Chemical analysis techniques and investigation of polycyclic aromatic hydrocarbons in fruit,vegetables and meats and their products[J].Food Chemistry,2019,277:156-161.
[7]Yan M,Nie H,Wang W,et al.Occurrence and toxicological risk assessment of polycyclic aromatic hydrocarbons and heavy metals in drinking water resources of Southern China[J].International Journal of Environmental Research and Public Health,2018,15(7),1422.
[8]Chen Y,Zhang J,Zhang F,et al.Polycyclic aromatic hydrocarbons in farmland soils around main reservoirs of Jilin Province,China:Occurrence,sources and potential human health risk[J].Environmental Geochemistry&Health,2017,40(2/3):1-12.
[9]Menzie C A,Potocki B B,Santodonato J.Exposure to carcinogenic PAHs in the environment[J].Environmental Science&Technology,1992,26:1278-1284.
[10]Jiang Y F,Wang X T,Wu M H,et al.Contamination,source identification,and risk assessment of polycyclic aromatic hydrocarbons in agricultural soil of Shanghai,China[J].Environmental Monitoring&Assessment,2011,183(1/2/3/4):139-150.
[11]Kuang S P,Wu Z C,Zhao L S.Accumulation and risk assessment of polycyclic aromatic hydrocarbons(PAHs)in soils around oil sludge in Zhongyuan oil field,China[J].Environmental Earth Sciences,2011,64(5):1353-1362.
[12]Nisbet C,Lagoy P.Toxic equivalency factors(TEFs)for polycyclic aromatic hydrocarbons(PAHs)[J].Reg Toxicol Pharmocol,1992,16(3):290-300.
[13]USEPA.Exposure factors handbook,Volume1:General factors[M].1997.
[14]Wand X T,Chen L,Wang X K,et al.Occurrence,sources and health risk assessment of polycyclic aromatic hydrocarbons in urban(Pudong)and suburban soils from Shanghai in China[J].Chemosphere,2015,119:1224-1232.
[15]范茜茜,史咲頔,邱兴华,等.二级热脱附结合气相色谱-质谱联用分析大气细颗粒物中多环芳烃类污染物[J].环境科学学报,2018,38(6):2304-2311.FAN Qian-qian,SHI Xiao-di,QIU Xing-hua,et al.Measurement of polycyclic aromatic hydrocarbons(PAHs)in ambient fine particulate matter using thermal desorption coupled with gas chromatographymass spectrometry[J].Acta Scientiae Circumstantiae,2018,38(6):2304-2311.
[16]李法云,胡成,张营,等.沈阳市街道灰尘中重金属的环境影响与健康风险评价[J].气象与环境学报,2010,26(6):59-64.LI Fa-yun,HU Cheng,ZHANG Ying,et al.Environmental impact and health risk assessment of heavy metals in street dust in Shenyang,Liaoning Province[J].Journal of Meteorology and Environment,2010,26(6):59-64.
[17]Jiang Y,Hu X,Yves U J,et al.Status,source and health risk assessment of polycyclic aromatic hydrocarbons in street dust of an industrial city,NW China[J].Ecotoxicology and Environmental Safety,2014,106:11-18.
[18]Bandowe B A,Nkansah M A.Occurrence,distribution and health risk from polycyclic aromatic compounds(PAHs,oxygenated-PAHs and azaarenes)in street dust from a major West African Metropolis[J].Science of the Total Environment,2016,553:439-449.
[19]Soltani N,Keshavarzi B,Moore F,et al.Ecological and human health hazards of heavy metals and polycyclic aromatic hydrocarbons(PAHs)in road dust of Isfahan metropolis,Iran[J].Science of the Total Environment,2014,505(6):712-723.
[20]Eleonora W,Dawn I,Rafaf K.Human health risk assessment,case study:An abandoned metal smelter site in Poland[J].Chemosphere,2002,47(5):507-515.
[21]Ferreira-Baptista L,Miguel E D.Geochemistry and risk assessment of street dust in Luanda,Angola:A tropical urban environment[J].Atmospheric Environment,2005,39(25):4501-4512.
[22]王喆,刘少卿,陈晓民,等.健康风险评价中中国人皮肤暴露面积的估算[J].安全与环境学报,2008,8(4):152-156.WANG Zhe,LIU Shao-qing,CHEN Xiao-min,et al.Estimates of the exposed dermal surface area of Chinese in view of human health risk assessment[J].Journal of Safety and Environment,2008,8(4):152-156.
[23]USEPA.Human health evaluation manual:Part A,Risk assessment guidance for superfund[EB/OL].[2010-10-8].http://www.epa.gov/oswer/riskassessment/ragsa/pdf/ch8.pdf.
[24]董继元,王式功,尚可政.黄河兰州段多环芳烃类有机污染物健康风险评价[J].农业环境科学学报,2009,28(9):1892-1897.DONG Ji-yuan,WANG Shi-gong,SHANG Ke-zheng.Water environmental health risk assessment of polycyclic aromatic hydrocarbons in the Lanzhou Reach of the Yellow River[J].Journal of Agro-Environment Science,2009,28(9):1892-1897.
[25]Zheng H,Qu C K,Zhang J Q,et al.Polycyclic aromatic hydrocarbons(PAHs)in agricultural soils from Ningde,China:Levels,sources,and human health risk assessment[J].Environmental Geochemistry and Health,DOI:10.1007/s10653-018-0188-7.
[26]Chen Y N,Zhang J Q,Zhang F,et al.Contamination and health risk assessment of PAHs in farmland soils of the Yinma River Basin,China[J].Ecotoxicology and Environmental Safety,2018,156:383-390.
[27]Nam J J,Thomas G O,Jaward F M,et al.PAHs in background soils from Western Europe:Influence of atmospheric deposition and soil organic matter[J].Chemosphere,2008,70(9):1596-1602.
[28]Nam J J,Song B H,Eom K C,et al.Distribution of polycyclic aromatic hydrocarbons in agricultural soils in South Korea[J].Chemosphere,2003,50:1281-1289.
[29]Chung M K,Hu R,Cheung K C,et al.Pollutants in Hong Kong soils:Polycyclic aromatic hydrocarbons[J].Chemosphere,2007,67(3):464-387473.
[30]Marquez-Bravo L G,Briggs D,Shayler H,et al.Concentrations of polycyclic aromatic hydrocarbons in New York City community garden soils:Potential sources and influential factors[J].Environmental Toxicology&Chemistry,2016,35(2):357-367.
[31]VROM.Environmental quality objectives in the Netherlands:A review of environmental quality objectives and their policy framework in the Netherlands[M].The Hague:Ministry of Housing,Spatial Planning and the Environment,1994.
[32]Yunker M B,Macdonald R W,et al.PAHs in the Fraser River basin:A critical appraisal of PAH ratios as indicators of PAH source and composition[J].Organic Geochemistry,2002,33(4):489-515.
[33]Rocher V,Azimi S,Régis M,et al.Hydrocarbons and heavy metals in the different sewer deposits in the‘Le Marais’catchment(Paris,France):Stocks,distributions and origins[J].Science of the Total Environment,2004,323(1/2/3):107-122.
[34]Lee B K,Dong T T T.Toxicity and source assignment of polycyclic aromatic hydrocarbons in road dust from urban residential and industrial areas in a typical industrial city in Korea[J].Journal of Material Cycles and Waste Management,2011,13(1):34-42.
[35]周玲莉,薛南冬,李发生,等.黄淮平原农田土壤中多环芳烃的分布、风险及来源[J].中国环境科学,2012,32(7):1250-1256.ZHOU Ling-li,XUE Nan-dong,LI Fa-sheng,et al.Distribution,source analysis and risk assessment of polycyclic aromatic hydrocarbons in farmland soils in Huanghuai Plain[J].China Environmental Science,2012,32(7):1250-1256.
[36]吴焕波.区域大气环境污染源人体健康风险评价方法研究[D].兰州:兰州大学,2016.WU Huan-bo.Study on human health risk assessment method for regional atmospheric environmental pollution sources[D].Lanzhou:Lanzhou University,2016.