加拿大阿萨巴斯卡地区Mildred泥炭柱多环芳烃分布特征及来源解析
|
摘要
利用气相色谱-质谱联用仪(GC-MS),对加拿大阿萨巴斯卡地区Mildred泥炭柱的35个泥炭样品的多环芳烃(polycyclic aromatic hydrocarbons,PAHs)浓度进行了测定,分析了其含量分布特征;采用特征比值和主成分分析-多元线性回归方法,解析PAHs的源。研究结果表明,泥炭样品中的PAHs以菲系列、二苯并噻吩系列、4环PAHs(荧蒽、芘、?)为主,萘系列及5环及以上PAHs含量偏低而难以被检测出来;泥炭柱中的PAHs含量为0.7～12.0μg/g,且随着深度的加深逐渐减少,其最大值出现在近地表处;泥炭柱中的PAHs主要是周边油砂工业活动排放造成,属于异地石油源,少部分PAHs源于化石燃料和木材燃烧,大气中的PAHs迁移和沉降是泥炭柱中的PAHs的主要输入途径;Mildred泥炭地中石油源的PAHs贡献率最大,所占比例为76.3%,化石燃料燃烧和树木燃烧排放的PAHs所占比例分别为12.9%和10.8%。
Polycyclic aromatic hydrocarbons(PAHs) in 35 peat samples collected from the Mildred peat core in the Athabasca Region, Canada, were quantitatively analyzed by gas chromatograph mass spectroscopy(GCMS). The distribution pattern of PAHs was discussed, and the PAHs source apportionment was conducted by characteristic ratio analysis and principal component analysis-multivariable linear regression. The results showed that many kinds of PAHs in peat samples were found, mainly including phenanthrene series, dibenzothiophene series, 4-rings PAHs(fluoranthene, pyrene, chrysene), whereas naphthalene series and 5-rings and above PAHs could not be detected because of low content. The concentrations of PAHs ranged between 0.7 μg/g and 12.0 μg/g, with gradually decreased trend with the depth. The maximum PAHs concentration occurred on or near the surface. PAHs deposition in the Mildred peat core was mainly caused by emissions from the surrounding oil sand industries, while a small portion of PAHs was derived from fossil fuel and wood combustions. Atmospheric migration and subsidence was the important pathway of the input of PAHs to the peat land.The primary source of PAHs was the petroleum source and its contribution rate was 76.3%. PAHs derived from fossil fuel combustion and wood combustion contributed up to12.9% and 10.8%, respectively.
Polycyclic aromatic hydrocarbons(PAHs) in 35 peat samples collected from the Mildred peat core in the Athabasca Region, Canada, were quantitatively analyzed by gas chromatograph mass spectroscopy(GCMS). The distribution pattern of PAHs was discussed, and the PAHs source apportionment was conducted by characteristic ratio analysis and principal component analysis-multivariable linear regression. The results showed that many kinds of PAHs in peat samples were found, mainly including phenanthrene series, dibenzothiophene series, 4-rings PAHs(fluoranthene, pyrene, chrysene), whereas naphthalene series and 5-rings and above PAHs could not be detected because of low content. The concentrations of PAHs ranged between 0.7 μg/g and 12.0 μg/g, with gradually decreased trend with the depth. The maximum PAHs concentration occurred on or near the surface. PAHs deposition in the Mildred peat core was mainly caused by emissions from the surrounding oil sand industries, while a small portion of PAHs was derived from fossil fuel and wood combustions. Atmospheric migration and subsidence was the important pathway of the input of PAHs to the peat land.The primary source of PAHs was the petroleum source and its contribution rate was 76.3%. PAHs derived from fossil fuel combustion and wood combustion contributed up to12.9% and 10.8%, respectively.
引文
[1]Wilcke W.Global patterns of polycyclic aromatic hydrocarbons(PAHs)in soil[J].Geoderma,2007,141141(3-4):157-166.
[2]王健,赵红梅,徐大伟,等.湿地生态系统中的多环芳烃研究进展[J].地球科学进展,2009,2424(8):936-941.
[3]王国平,贾琳,刘景双,等.国外大气沉降泥炭沼泽档案研究进展[J].湿地科学,2006,44(1):69-74.
[4]赵红梅,王健,于晓菲,等.三江平原沼泽土中多环芳烃分布及火烧的影响[J].湿地科学,2010,88(1):43-47.
[5]Berset J D,Kuehne P,Shotyk W.Concentrations and distribution of some polychlorinated biphenyls(PCBs)and polycyclic aromatic hydrocarbons(PAHs)in an ombrotrophic peat bog profile of Switzerland[J].Science of the Total Environment,2001,267(1-3):67-85.
[6]Malawska M,Bojakowska I,Wi?komirski B.Polycyclic aromatic hydrocarbons(PAHs)in peat and plants from selected peat-bogs in the northeast of Poland[J].Journal of Plant Nutrition and Soil Science,2002,165165(6):686-691.
[7]Zhang Y,Shotyk W,Zaccone C,et al.Airborne petcoke dust is a major source of polycyclic aromatic hydrocarbons in the Athabasca Oil Sands Region[J].Environmental Science&Technology,2016,5050(4):1711-1720.
[8]Bari M A,Kindzierski W B,Cho S.A wintertime investigation of atmospheric deposition of metals and polycyclic aromatic hydrocarbons in the Athabasca Oil Sands Region,Canada[J].Science of the Total Environment,2014,485485-486(3):180-192.
[9]Jautzy J J,Ahad J M,Hall R I,et al.Source apportionment of background PAHs in the Peace-Athabasca Delta(Alberta,Canada)using molecular level radiocarbon analysis[J].Environmental Science&Technology,2015,4949(15):9056-63.
[10]Kelly E N,Short J W,Schindler D W,et al.Oil sands development contributes polycyclic aromatic compounds to the Athabasca River and its tributaries[J].Proceedings of the National Academy of Sciences,2009,106106(52):22346-22351.
[11]史彩奎,贾益群,王国平.长白山雨养泥炭表层多环芳烃组成分布及来源分析[J].中国环境科学,2008,2828(5):385-388.
[12]明荔莉,李军,刘向,等.若尔盖草原泥炭柱中多环芳烃的沉积记录[J].第四纪研究,2010,3030(6):1145-1150.
[13]杨佩华,韩彬,崔志松,等.石油平台周边海域多环芳烃的分布特征、源解析及风险评估[J].环境化学,2016,3535(1):170-179.
[14]Magnan G,Bellen S V,Davies L,et al.Impact of the Little Ice Age cooling and 20th century climate change on peatland vegetation dynamics in central and northern Alberta using a multiproxy approach and high-resolution peat chronologies[J].Quaternary Science Reviews,2018,185185:230-243.
[15]Christensen E R,Arora S.Source apportionment of PAHs in sediments using factor analysis by time records:application to Lake Michigan,USA[J].Water Research,2007,4141(1):168-176.
[16]史彩奎,贾益群,王国平.大兴安岭摩天岭雨养泥炭沼泽多环芳烃分布特征与来源分析[J].湿地科学,2007,55(3):260-265.
[17]杜芳芳,杨毅,刘敏,等.上海市表层土壤中多环芳烃的分布特征与源解析[J].中国环境科学,2014,344(4):989-995.
[18]李嘉康,宋雪英,崔小维,等.土壤中多环芳烃源解析技术研究进展[J].生态科学,2017,3636(5):223-231.
[19]陈锋,孟凡生,王业耀,等.基于主成分分析-多元线性回归的松花江水体中多环芳烃源解析[J].中国环境监测,2016,3232(4):49-53.
[20]张生银,李双林,董贺平,等.南黄海中部表层沉积物中多环芳烃分布特征及来源分析[J].中国环境科学,2013,3333(7):1263-1270.
[21]Yunker M B,Macdonald R W,Goyette D,et al.Natural and anthropogenic inputs of hydrocarbons to the Strait of Georgia[J].Science of the Total Environment,1999,22525(3):181-209.
[22]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,2002,3333(4):489-515.
[23]HuangH,BowlerBFJ,OldenburgTBP,et al.The effect of biodegradation on polycyclic aromatic hydrocarbons in reservoired oils from the Liaohe basin,NE China[J].Organic Geochemistry,2004,3535(11-12):1619-1634.
[24]Radke M,Welte D H.The methylphenanthrene index(MPI):a maturity parameter based on aromatic hydrocarbons[J].Advances in Organic Geochemistry,1981,19831983:504-512.
[25]Yang C,Wang Z,Yang Z,et al.Chemical fingerprints of Alberta oil sands and related petroleum products[J].Environmental Forensics,2011,1212(2):173-188.
[26]Chakhmakhchev A,Suzuki M,Takayama K.Distribution of alkylated dibenzothiophenes in petroleum as a tool for maturity assessments[J].Organic Geochemistry,1997,2626(7-8):483-489.
[27]罗健,程克明,付立新,等.烷基二苯并噻吩-烃源岩热演化新指标[J].石油学报,2001,2222(3):27-31.
[28]Ramdahl T.Retene-a molecular marker of wood combustion in ambient air[J].Nature,1983,306306(5943):580-582.
[2]王健,赵红梅,徐大伟,等.湿地生态系统中的多环芳烃研究进展[J].地球科学进展,2009,2424(8):936-941.
[3]王国平,贾琳,刘景双,等.国外大气沉降泥炭沼泽档案研究进展[J].湿地科学,2006,44(1):69-74.
[4]赵红梅,王健,于晓菲,等.三江平原沼泽土中多环芳烃分布及火烧的影响[J].湿地科学,2010,88(1):43-47.
[5]Berset J D,Kuehne P,Shotyk W.Concentrations and distribution of some polychlorinated biphenyls(PCBs)and polycyclic aromatic hydrocarbons(PAHs)in an ombrotrophic peat bog profile of Switzerland[J].Science of the Total Environment,2001,267(1-3):67-85.
[6]Malawska M,Bojakowska I,Wi?komirski B.Polycyclic aromatic hydrocarbons(PAHs)in peat and plants from selected peat-bogs in the northeast of Poland[J].Journal of Plant Nutrition and Soil Science,2002,165165(6):686-691.
[7]Zhang Y,Shotyk W,Zaccone C,et al.Airborne petcoke dust is a major source of polycyclic aromatic hydrocarbons in the Athabasca Oil Sands Region[J].Environmental Science&Technology,2016,5050(4):1711-1720.
[8]Bari M A,Kindzierski W B,Cho S.A wintertime investigation of atmospheric deposition of metals and polycyclic aromatic hydrocarbons in the Athabasca Oil Sands Region,Canada[J].Science of the Total Environment,2014,485485-486(3):180-192.
[9]Jautzy J J,Ahad J M,Hall R I,et al.Source apportionment of background PAHs in the Peace-Athabasca Delta(Alberta,Canada)using molecular level radiocarbon analysis[J].Environmental Science&Technology,2015,4949(15):9056-63.
[10]Kelly E N,Short J W,Schindler D W,et al.Oil sands development contributes polycyclic aromatic compounds to the Athabasca River and its tributaries[J].Proceedings of the National Academy of Sciences,2009,106106(52):22346-22351.
[11]史彩奎,贾益群,王国平.长白山雨养泥炭表层多环芳烃组成分布及来源分析[J].中国环境科学,2008,2828(5):385-388.
[12]明荔莉,李军,刘向,等.若尔盖草原泥炭柱中多环芳烃的沉积记录[J].第四纪研究,2010,3030(6):1145-1150.
[13]杨佩华,韩彬,崔志松,等.石油平台周边海域多环芳烃的分布特征、源解析及风险评估[J].环境化学,2016,3535(1):170-179.
[14]Magnan G,Bellen S V,Davies L,et al.Impact of the Little Ice Age cooling and 20th century climate change on peatland vegetation dynamics in central and northern Alberta using a multiproxy approach and high-resolution peat chronologies[J].Quaternary Science Reviews,2018,185185:230-243.
[15]Christensen E R,Arora S.Source apportionment of PAHs in sediments using factor analysis by time records:application to Lake Michigan,USA[J].Water Research,2007,4141(1):168-176.
[16]史彩奎,贾益群,王国平.大兴安岭摩天岭雨养泥炭沼泽多环芳烃分布特征与来源分析[J].湿地科学,2007,55(3):260-265.
[17]杜芳芳,杨毅,刘敏,等.上海市表层土壤中多环芳烃的分布特征与源解析[J].中国环境科学,2014,344(4):989-995.
[18]李嘉康,宋雪英,崔小维,等.土壤中多环芳烃源解析技术研究进展[J].生态科学,2017,3636(5):223-231.
[19]陈锋,孟凡生,王业耀,等.基于主成分分析-多元线性回归的松花江水体中多环芳烃源解析[J].中国环境监测,2016,3232(4):49-53.
[20]张生银,李双林,董贺平,等.南黄海中部表层沉积物中多环芳烃分布特征及来源分析[J].中国环境科学,2013,3333(7):1263-1270.
[21]Yunker M B,Macdonald R W,Goyette D,et al.Natural and anthropogenic inputs of hydrocarbons to the Strait of Georgia[J].Science of the Total Environment,1999,22525(3):181-209.
[22]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,2002,3333(4):489-515.
[23]HuangH,BowlerBFJ,OldenburgTBP,et al.The effect of biodegradation on polycyclic aromatic hydrocarbons in reservoired oils from the Liaohe basin,NE China[J].Organic Geochemistry,2004,3535(11-12):1619-1634.
[24]Radke M,Welte D H.The methylphenanthrene index(MPI):a maturity parameter based on aromatic hydrocarbons[J].Advances in Organic Geochemistry,1981,19831983:504-512.
[25]Yang C,Wang Z,Yang Z,et al.Chemical fingerprints of Alberta oil sands and related petroleum products[J].Environmental Forensics,2011,1212(2):173-188.
[26]Chakhmakhchev A,Suzuki M,Takayama K.Distribution of alkylated dibenzothiophenes in petroleum as a tool for maturity assessments[J].Organic Geochemistry,1997,2626(7-8):483-489.
[27]罗健,程克明,付立新,等.烷基二苯并噻吩-烃源岩热演化新指标[J].石油学报,2001,2222(3):27-31.
[28]Ramdahl T.Retene-a molecular marker of wood combustion in ambient air[J].Nature,1983,306306(5943):580-582.