种植油麦菜评价多环芳烃污染土壤的农用风险
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摘要
污染土壤引起的农产品安全问题已不容忽视.为了探讨多环芳烃(polycyclic aromatic hydrocarbons,PAHs)污染土壤农用的安全性,本文通过盆栽实验方法,以某焦化企业周边长期受PAHs污染的农田土壤为研究对象,以广泛种植的油麦菜(Lactuca sativa L.)为农产品代表,利用超声振荡提取和气相色谱-质谱联用仪(GC-MS)分析方法,解析样品中优先控制的16种PAHs的含量,揭示土壤-油麦菜体系中PAHs的迁移转化与富集特征,评估其潜在风险.结果表明,油麦菜地上部分(YS)PAHs的含量(Σ16PAHs)大于地下部分(GS),YS中3～5环PAHs相对含量高,GS中4～6环PAHs含量高. YS对不同PAHs的富集系数均大于GS,YS中蒽(Ant)的富集系数最大(2. 41),荧蒽(Fla)最小(0. 458),GS中苯并[a]芘(Bap)最大(0. 862),Fla最小(0. 130). 16种PAHs从GS到YS的转运系数均大于1. 00.关联性分析表明GS与初始土壤(SS) PAHs拟合优度中等(R~2=0. 71),YS与SS的PAHs拟合优度最大(R~2=1. 0),YS和GS的PAHs拟合优度最小(R~2=0. 39). YS和GS的健康风险值分别是国家食品标准Bap最大风险控制值的11. 8和12. 7倍.表明油麦菜食用的潜在风险较高,焦化企业周边污染土壤农用的安全问题不容忽视.
In order to evaluate the potential agricultural risks of soil contaminated by polycyclic aromatic hydrocarbons( PAHs),Lactuca sativa L. was used as a model leaf vegetable plant to investigate the enrichment characteristics of PAHs in the different tissues of Lactuca sativa L,such as its underground parts( GS) and aboveground parts( YS),which were studied through an experiment involving potted cultivation in PAHs contaminated soil that was taken from the agricultural soil around a coking enterprise area. The concentrations of the different PAHs in the soil and plant tissues were analyzed using ultrasonic oscillation extraction and highperformance liquid chromatography-mass spectrometry( GC-MS) analysis methods. The results show that the enrichment of the total PAHs( Σ 16 PAHs) in the YS is higher than that in the GS. The components enriched in the YS mainly consist of 3-5 ring PAHs,and those in the GS consist of 4-6 ring PAHs. The coefficients of the different PAHs enriched in the YS were higher than those of the GS. The enrichment coefficient of anthracene( Ant) was the largest and that of fluoranthene( Fla) was the smallest in the YS,while the enrichment coefficient of benzene[a]pyre( Bap) was the largest and that of Fla was the smallest in the GS. The transfer coefficients of the different PAHs from the GS to the YS were greater than the rate from the initial soil( SS) to the GS; the value is less than 1 from the SS to GS. The correlations and goodness of fit were analyzed for the concentrations of PAHs in the SS,GS and YS. TheΣ 16 PAHs in the SS showed positive correlations with the Σ 16 PAHs in the YS and in GS. The goodness of fit of the correlation of the PAHs in YS to those in the SS was the largest( R~2= 1. 0),while the goodness-of-fit for the correlation between the GS and SS was lower( R~2= 0. 71). The benzo[a]pyrene equivalent concentration values( Σ 16 PAHsBapeq) of YS and GS were 11. 8 and 12. 7 times the maximum value of Bap level allowed in food. The study indicates that contaminated farmland soil would present a high health risk when it was used to grow the plant.
In order to evaluate the potential agricultural risks of soil contaminated by polycyclic aromatic hydrocarbons( PAHs),Lactuca sativa L. was used as a model leaf vegetable plant to investigate the enrichment characteristics of PAHs in the different tissues of Lactuca sativa L,such as its underground parts( GS) and aboveground parts( YS),which were studied through an experiment involving potted cultivation in PAHs contaminated soil that was taken from the agricultural soil around a coking enterprise area. The concentrations of the different PAHs in the soil and plant tissues were analyzed using ultrasonic oscillation extraction and highperformance liquid chromatography-mass spectrometry( GC-MS) analysis methods. The results show that the enrichment of the total PAHs( Σ 16 PAHs) in the YS is higher than that in the GS. The components enriched in the YS mainly consist of 3-5 ring PAHs,and those in the GS consist of 4-6 ring PAHs. The coefficients of the different PAHs enriched in the YS were higher than those of the GS. The enrichment coefficient of anthracene( Ant) was the largest and that of fluoranthene( Fla) was the smallest in the YS,while the enrichment coefficient of benzene[a]pyre( Bap) was the largest and that of Fla was the smallest in the GS. The transfer coefficients of the different PAHs from the GS to the YS were greater than the rate from the initial soil( SS) to the GS; the value is less than 1 from the SS to GS. The correlations and goodness of fit were analyzed for the concentrations of PAHs in the SS,GS and YS. TheΣ 16 PAHs in the SS showed positive correlations with the Σ 16 PAHs in the YS and in GS. The goodness of fit of the correlation of the PAHs in YS to those in the SS was the largest( R~2= 1. 0),while the goodness-of-fit for the correlation between the GS and SS was lower( R~2= 0. 71). The benzo[a]pyrene equivalent concentration values( Σ 16 PAHsBapeq) of YS and GS were 11. 8 and 12. 7 times the maximum value of Bap level allowed in food. The study indicates that contaminated farmland soil would present a high health risk when it was used to grow the plant.
引文
[1]Jiao H H,Bian G P,Chen X,et al.Distribution,sources,and potential risk of polycyclic aromatic hydrocarbons in soils from an industrial district in Shanxi,China[J].Environmental Science and Pollution Research,2017,24(13):12243-12260.
[2]Jiao H H,Wang,Q,Zhao N N,et al.Distributions and sources of polycyclic aromatic hydrocarbons(PAHs)in soils around a chemical plant in Shanxi,China[J].International Journal of Environmental Research and Public Health,2017,14(10):1198.
[3]Duan Y H,Shen G F,Tao S,et al.Characteristics of polycyclic aromatic hydrocarbons in agricultural soils at a typical coke production base in Shanxi,China[J].Chemosphere,2015,127:64-69.
[4]National Academy of Sciences.Report of the committee on research advisory to the U.S.department of agriculture[R].Washington,DC:National Academy Press,1972.
[5]International Agency for Research on Cancer(IARC).Monographs on the evaluation of the carcinogenic risk of chemicals to humans.Polynuclear aromatic compounds,part 1,chemical,environmental,and experimental data[M].Lyon,France:IARC,1983.95-275.
[6]Lyon(France)International Agency for Research on Cancer.IARC monographs on the evaluation of the carcinogenic risk of chemicals to humans:international Agency for Research on Cancer.Lyon,1986[J].Food and Chemical Toxicology,1987,25(9):717.
[7]Maliszewska-Kordybach B.Polycyclic aromatic hydrocarbons in agricultural soils in Poland:preliminary proposals for criteria to evaluate the level of soil contamination[J].Applied Geochemistry,1996,11(1-2):121-127.
[8]Amador-Mu1oz O,Bazán-Torija S,Villa-Ferreira S A,et al.Opposing seasonal trends for polycyclic aromatic hydrocarbons and PM10:health risk and sources in southwest Mexico City[J].Atmospheric Research,2013,122:199-212.
[9]Jiao H H,Rui X P,Wu S H,et al.Polycyclic aromatic hydrocarbons in the Dagang Oilfield(China):distribution,sources,and risk assessment[J].International Journal of Environmental Research and Public Health,2015,12(6):5775-5791.
[10]De Nicola F,Maisto G,Prati M V,et al.Leaf accumulation of trace elements and polycyclic aromatic hydrocarbons(PAHs)in Quercus ilex L.[J].Environmental Pollution,2008,153(2):376-383.
[11]周婕成,毕春娟,陈振楼,等.温州城市河流河岸带土壤中PAHs的污染特征与来源[J].环境科学,2012,33(12):4237-4243.Zhou J C,Bi C J,Chen Z L,et al.Pollution characteristics and sources of polycyclic aromatic hydrocarbons in riparian soils along urban rivers of Wenzhou city[J].Environmental Science,2012,33(12):4237-4243.
[12]US EPA.Health effects assessments for polycyclic aromatic hydrocarbons(PAHs)[R].EPA 549/1-86-013,Cincinnati:US Environmental Protection Agency(EPA),Environmental Criteria and Assessment Office,1984.
[13]Nisbet I C T,Lagoy P K.Toxic equivalency factors(TEFs)for polycyclic aromatic hydrocarbons(PAHs)[J].Regulatory Toxicology and Pharmacology,1992,16(3):290-300.
[14]Yunker M B,Macdonald R W,Vingarzan R,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.
[15]Galarneau E.Source specificity and atmospheric processing of airborne PAHs:implications for source apportionment[J].Atmospheric Environment,2008,42(35):8139-8149.
[16]张天彬,万洪富,杨国义,等.珠江三角洲典型城市农业土壤及蔬菜中的多环芳烃分布[J].环境科学学报,2008,28(11):2375-2384.Zhang T B,Wan H F,Yang G Y,et al.Distribution of polycyclic aromatic hydrocarbons in agricultural soil and vegetables of Foshan City in the Pearl River Delta[J].Acta Scientiae Circumstantiae,2008,28(11):2375-2384.
[17]万开,江明,杨国义,等.珠江三角洲典型城市蔬菜中多环芳烃分布特征[J].土壤,2009,41(4):583-587.Wan K,Jiang M,Yang G Y,et al.Distribution characteristics of PAHs in vegetables of typical city in Pearl River Delta-A case study of Dongguan City[J].Soils,2009,41(4):583-587.
[18]Li Y T,Li F B,Chen J J,et al.The concentrations,distribution and sources of PAHs in agricultural soils and vegetables from Shunde,Guangdong,China[J].Environmental Monitoring and Assessment,2008,139(1-3):61-76.
[19]尹春芹,蒋新,杨兴伦,等.施肥对花红苋菜吸收和积累土壤中PAHs的影响[J].环境科学,2008,28(8):742-747.Yin C Q,Jiang X,Yang X L,et al.Influence of fertilization on flower red amaranth uptake and accumulation of PAHs in soil[J].Environmental Science,2008,28(8):742-747.
[20]崔阳,郭利利,张桂香,等.山西焦化污染区土壤和农产品中PAHs风险特征初步研究[J].农业环境科学学报,2015,34(1):72-79.Cui Y,Guo L L,Zhang G X,et al.Human health risks of PAHs in soils and agricultural products in coking areas,Shanxi province,China[J].Journal of Agro-Environment Science,2015,34(1):72-79.
[21]沈菲.钢铁工业区农田植物PAHs的浓度水平和影响因素[D].杭州:浙江大学,2006.Shen F.THE concentration and distribution of polycyclic aromatic hydrocarbons in plants in an iron and steel industrial area[D].Hangzhou:Zhejiang University,2006.
[22]Sun L,Liao X Y,Yan X L,et al.Evaluation of heavy metal and polycyclic aromatic hydrocarbons accumulation in plants from typical industrial sites:potential candidate in phytoremediation for co-contamination[J].Environmental Science and Pollution Research International,2014,21(21):12494-12504.
[23]王海翠,胡林林,李敏,等.多环芳烃(PAHs)对油菜生长的影响及其积累效应[J].植物生态学报,2013,37(12):1123-1131.
[24]梁宵,占新华,周立祥.不同作物根系多环芳烃吸收特征差异的比较研究[J].环境科学,2012,33(7):2516-2521.Liang X,Zhan X L,Zhou L X.Characterization comparison of polycyclic aromatic hydrocarbon uptake by roots of different crops[J].Environmental Science,2012,33(7):2516-2521.
[25]蓝家程,孙玉川,肖时珍.多环芳烃在岩溶地下河表层沉积物-水相的分配[J].环境科学,2015,36(11):4081-4087.Lan J C,Sun Y C,Xiao S Z.Water-Sediment partition of polycyclic aromatic hydrocarbons in Karst underground river[J].Enviromental Science,2015,36(11):4081-4087.
[26]王戎,何杞双,王雁,等.可溶性有机物对玉米根部菲与芴吸着与吸收过程的影响[J].农业环境科学学报,2009,28(1):35-39.Wang R,He Q S,Wang Y,et al.Impact of dissolved organic matter on sorption and absorption of fluorene and phenanthrene to maize root[J].Journal of Agro-Environment Science,2009,28(1):35-39.
[27]Moeckel C,Thomas G O,Barber J H,et al.Uptake and storage of PCBs by plant cuticles[J].Environment Science&Technology,2008,42(1):100-105.
[28]焦海华,张淑珍,景旭东,等.油田区多环芳烃污染盐碱土壤活性微生物群落结构解析[J].生态学报,2016,36(21):6994-7005.Jiao H H,Zhang S Z,Jing X D,et al.Analysis of the structure and distribution characteristics of the microbial community in saline-alkali soil contaminated with polycyclic aromatic hydrocarbons[J].Acta Ecologica Sinica,2016,36(21):6994-7005.
[29]GB 2762-2017,食品安全国家标准食品中污染物限量[S].
[2]Jiao H H,Wang,Q,Zhao N N,et al.Distributions and sources of polycyclic aromatic hydrocarbons(PAHs)in soils around a chemical plant in Shanxi,China[J].International Journal of Environmental Research and Public Health,2017,14(10):1198.
[3]Duan Y H,Shen G F,Tao S,et al.Characteristics of polycyclic aromatic hydrocarbons in agricultural soils at a typical coke production base in Shanxi,China[J].Chemosphere,2015,127:64-69.
[4]National Academy of Sciences.Report of the committee on research advisory to the U.S.department of agriculture[R].Washington,DC:National Academy Press,1972.
[5]International Agency for Research on Cancer(IARC).Monographs on the evaluation of the carcinogenic risk of chemicals to humans.Polynuclear aromatic compounds,part 1,chemical,environmental,and experimental data[M].Lyon,France:IARC,1983.95-275.
[6]Lyon(France)International Agency for Research on Cancer.IARC monographs on the evaluation of the carcinogenic risk of chemicals to humans:international Agency for Research on Cancer.Lyon,1986[J].Food and Chemical Toxicology,1987,25(9):717.
[7]Maliszewska-Kordybach B.Polycyclic aromatic hydrocarbons in agricultural soils in Poland:preliminary proposals for criteria to evaluate the level of soil contamination[J].Applied Geochemistry,1996,11(1-2):121-127.
[8]Amador-Mu1oz O,Bazán-Torija S,Villa-Ferreira S A,et al.Opposing seasonal trends for polycyclic aromatic hydrocarbons and PM10:health risk and sources in southwest Mexico City[J].Atmospheric Research,2013,122:199-212.
[9]Jiao H H,Rui X P,Wu S H,et al.Polycyclic aromatic hydrocarbons in the Dagang Oilfield(China):distribution,sources,and risk assessment[J].International Journal of Environmental Research and Public Health,2015,12(6):5775-5791.
[10]De Nicola F,Maisto G,Prati M V,et al.Leaf accumulation of trace elements and polycyclic aromatic hydrocarbons(PAHs)in Quercus ilex L.[J].Environmental Pollution,2008,153(2):376-383.
[11]周婕成,毕春娟,陈振楼,等.温州城市河流河岸带土壤中PAHs的污染特征与来源[J].环境科学,2012,33(12):4237-4243.Zhou J C,Bi C J,Chen Z L,et al.Pollution characteristics and sources of polycyclic aromatic hydrocarbons in riparian soils along urban rivers of Wenzhou city[J].Environmental Science,2012,33(12):4237-4243.
[12]US EPA.Health effects assessments for polycyclic aromatic hydrocarbons(PAHs)[R].EPA 549/1-86-013,Cincinnati:US Environmental Protection Agency(EPA),Environmental Criteria and Assessment Office,1984.
[13]Nisbet I C T,Lagoy P K.Toxic equivalency factors(TEFs)for polycyclic aromatic hydrocarbons(PAHs)[J].Regulatory Toxicology and Pharmacology,1992,16(3):290-300.
[14]Yunker M B,Macdonald R W,Vingarzan R,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.
[15]Galarneau E.Source specificity and atmospheric processing of airborne PAHs:implications for source apportionment[J].Atmospheric Environment,2008,42(35):8139-8149.
[16]张天彬,万洪富,杨国义,等.珠江三角洲典型城市农业土壤及蔬菜中的多环芳烃分布[J].环境科学学报,2008,28(11):2375-2384.Zhang T B,Wan H F,Yang G Y,et al.Distribution of polycyclic aromatic hydrocarbons in agricultural soil and vegetables of Foshan City in the Pearl River Delta[J].Acta Scientiae Circumstantiae,2008,28(11):2375-2384.
[17]万开,江明,杨国义,等.珠江三角洲典型城市蔬菜中多环芳烃分布特征[J].土壤,2009,41(4):583-587.Wan K,Jiang M,Yang G Y,et al.Distribution characteristics of PAHs in vegetables of typical city in Pearl River Delta-A case study of Dongguan City[J].Soils,2009,41(4):583-587.
[18]Li Y T,Li F B,Chen J J,et al.The concentrations,distribution and sources of PAHs in agricultural soils and vegetables from Shunde,Guangdong,China[J].Environmental Monitoring and Assessment,2008,139(1-3):61-76.
[19]尹春芹,蒋新,杨兴伦,等.施肥对花红苋菜吸收和积累土壤中PAHs的影响[J].环境科学,2008,28(8):742-747.Yin C Q,Jiang X,Yang X L,et al.Influence of fertilization on flower red amaranth uptake and accumulation of PAHs in soil[J].Environmental Science,2008,28(8):742-747.
[20]崔阳,郭利利,张桂香,等.山西焦化污染区土壤和农产品中PAHs风险特征初步研究[J].农业环境科学学报,2015,34(1):72-79.Cui Y,Guo L L,Zhang G X,et al.Human health risks of PAHs in soils and agricultural products in coking areas,Shanxi province,China[J].Journal of Agro-Environment Science,2015,34(1):72-79.
[21]沈菲.钢铁工业区农田植物PAHs的浓度水平和影响因素[D].杭州:浙江大学,2006.Shen F.THE concentration and distribution of polycyclic aromatic hydrocarbons in plants in an iron and steel industrial area[D].Hangzhou:Zhejiang University,2006.
[22]Sun L,Liao X Y,Yan X L,et al.Evaluation of heavy metal and polycyclic aromatic hydrocarbons accumulation in plants from typical industrial sites:potential candidate in phytoremediation for co-contamination[J].Environmental Science and Pollution Research International,2014,21(21):12494-12504.
[23]王海翠,胡林林,李敏,等.多环芳烃(PAHs)对油菜生长的影响及其积累效应[J].植物生态学报,2013,37(12):1123-1131.
[24]梁宵,占新华,周立祥.不同作物根系多环芳烃吸收特征差异的比较研究[J].环境科学,2012,33(7):2516-2521.Liang X,Zhan X L,Zhou L X.Characterization comparison of polycyclic aromatic hydrocarbon uptake by roots of different crops[J].Environmental Science,2012,33(7):2516-2521.
[25]蓝家程,孙玉川,肖时珍.多环芳烃在岩溶地下河表层沉积物-水相的分配[J].环境科学,2015,36(11):4081-4087.Lan J C,Sun Y C,Xiao S Z.Water-Sediment partition of polycyclic aromatic hydrocarbons in Karst underground river[J].Enviromental Science,2015,36(11):4081-4087.
[26]王戎,何杞双,王雁,等.可溶性有机物对玉米根部菲与芴吸着与吸收过程的影响[J].农业环境科学学报,2009,28(1):35-39.Wang R,He Q S,Wang Y,et al.Impact of dissolved organic matter on sorption and absorption of fluorene and phenanthrene to maize root[J].Journal of Agro-Environment Science,2009,28(1):35-39.
[27]Moeckel C,Thomas G O,Barber J H,et al.Uptake and storage of PCBs by plant cuticles[J].Environment Science&Technology,2008,42(1):100-105.
[28]焦海华,张淑珍,景旭东,等.油田区多环芳烃污染盐碱土壤活性微生物群落结构解析[J].生态学报,2016,36(21):6994-7005.Jiao H H,Zhang S Z,Jing X D,et al.Analysis of the structure and distribution characteristics of the microbial community in saline-alkali soil contaminated with polycyclic aromatic hydrocarbons[J].Acta Ecologica Sinica,2016,36(21):6994-7005.
[29]GB 2762-2017,食品安全国家标准食品中污染物限量[S].
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