长江口大气多氯联苯干湿沉降通量
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摘要
大气干、湿沉降是水体持久性有机污染物的主要来源.长江口是我国陆海相互作用研究的关键区域,是大气污染物监测的重点区域.为了解长江口大气中多氯联苯(Polychlorinated Biphenyls, PCBs)的污染特征,本研究共采集了自2013年10月—2014年8月4个季度93对大气样品(气态和颗粒态)和13个雨水样品,分析了样品中7种典型PCBs浓度并估算了PCBs的干、湿沉降通量.结果表明:①长江口大气中PCBs(气态和颗粒态)浓度范围是2.37～207 pg·m~(-3),平均浓度为44.9 pg·m~(-3);与以海洋为背景的国内外大气中PCBs相比,浓度处于中度水平;大气中PCBs主要存在于气态中,占77%;夏季气态PCBs浓度明显高于其他3个季度;颗粒态PCBs浓度呈冬、春季高,夏、秋季低的特点.②PCBs的干沉降通量为681～2330 pg·m~(-2)·d~(-1),年均值为1880 pg·m~(-2)·d~(-1),冬、春季干沉降通量明显高于夏、秋季;湿沉降通量为184～1210 pg·m~(-2)·d~(-1),年均值为863 pg·m~(-2)·d~(-1),夏季湿沉降通量明显低于其他3个季节.总体上,PCBs干、湿沉降通量年均变化为865～3300 pg·m~(-2)·d~(-1),年均值为2250 pg·m~(-2)·d~(-1),干沉降占总沉降通量的69%.
Atmospheric dry and wet depositions are important sources of persistent organic pollutants(POPs) to water. The Yangtze River Estuary is an important area for researches of air pollution and land-sea interactions. Ninety three air samples(gaseous and particle phases) and thirteen precipitation samples were collected from October 2013 to August 2014 over the Yangtze River Estuary to analyze seven PCBs. The results showed that:①The total concentrations of PCBs ranged from 2.37 to 207 pg·m~(-3), with average value of 44.9 pg·m~(-3). Compared with other domestic and oversea areas, the total concentrations of PCBs over the Yangtze River Estuary were at the middle levels. PCBs mainly distributed in the gaseous phase accounting for 77% of total concentrations. The concentrations of PCBs showed seasonal variations. Higher concentrations were found in summer than other seasons in gaseous phase, while, in particle phase, higher concentrations were found in winter. ②The dry deposition fluxes of PCBs ranged from 681 to 2330 pg·m~(-2)·d~(-1) with the average value of 1880 pg·m~(-2)·d~(-1). The wet deposition fluxes of PCBs ranged from 184 to 1210 pg·m~(-2)·d~(-1) and the annual average was 863 pg·m~(-2)·d~(-1). The total deposition fluxes of PCBs ranged from 865～3300 pg·m~(-2)·d~(-1), and the average annual value was 2250 pg·m~(-2)·d~(-1). The dry deposition fluxes accounted for 69% of total deposition fluxes.
Atmospheric dry and wet depositions are important sources of persistent organic pollutants(POPs) to water. The Yangtze River Estuary is an important area for researches of air pollution and land-sea interactions. Ninety three air samples(gaseous and particle phases) and thirteen precipitation samples were collected from October 2013 to August 2014 over the Yangtze River Estuary to analyze seven PCBs. The results showed that:①The total concentrations of PCBs ranged from 2.37 to 207 pg·m~(-3), with average value of 44.9 pg·m~(-3). Compared with other domestic and oversea areas, the total concentrations of PCBs over the Yangtze River Estuary were at the middle levels. PCBs mainly distributed in the gaseous phase accounting for 77% of total concentrations. The concentrations of PCBs showed seasonal variations. Higher concentrations were found in summer than other seasons in gaseous phase, while, in particle phase, higher concentrations were found in winter. ②The dry deposition fluxes of PCBs ranged from 681 to 2330 pg·m~(-2)·d~(-1) with the average value of 1880 pg·m~(-2)·d~(-1). The wet deposition fluxes of PCBs ranged from 184 to 1210 pg·m~(-2)·d~(-1) and the annual average was 863 pg·m~(-2)·d~(-1). The total deposition fluxes of PCBs ranged from 865～3300 pg·m~(-2)·d~(-1), and the average annual value was 2250 pg·m~(-2)·d~(-1). The dry deposition fluxes accounted for 69% of total deposition fluxes.
引文
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Mi H H,Wu Z S,Lin L F,et al.2012.Atmospheric dry deposition of polychlorinated dibenzo-p-dioxins/dibenzofurans (PCDD/Fs) and polychlorinated biphenyls(PCBs) in Southern Taiwan[J].Aerosol and Air Quality Research,12:1016-1029
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Mustafa O,Banu C,Eylem D,et al.2008.Air-water exchange of polychlorinated biphenyls (PCBs) and organochlorine pesticides (OCPs) at a coastal site in Izmir Bay,Turkey[J].Marine Chemistry,109(1/2):115-129
Odabasi M,Cetin B,Demircioglu E,et al.2008.Air-water exchange of polychlorinated biphenyls (PCBs) and organochlorine pesticides (OCPs) at a coastal site in Izmir Bay,Turkey[J].Marine Chemistry,109(1/2):115-129
Simcik M F,Basu I,Sweet C W,et al.1999.Temperature dependence and temporal trends of polychlorinated biphenyl congener in the Great Lakes atmosphere[J].Environmental Science and Technology,33(12):1991-1995
Simcik M F,Zhang H,Eisenreich S J,et al.1997.Urban contamination of the Chicago/Coastal Lake Michigan atmosphere by PCBs and PAHs during AEOLOS[J].Environmental Science and Technology,31(7):2141-2147
王飞,2015.持久性有机污染物多氯联苯(PCBs)的研究进展[J].科技资讯,(20):139-143
Wania F,Haugen J E,Lei Y D,et al.1998.Temperature dependence of atmospheric concentrations of semivolatile organic compounds[J].Environmental Science & Technology,32:1013-1021
杨国胜,马玲玲,许殿斗,等,2012.北京市石景山区夏季雨水和大气中PCBs的特征解析[J].中国环境科学,32(7):1234-1240
Yue Q,Zhang K,Zhang B Z,et al.2011.Occurrence,phase distribution and depositional intensity of dichlorodiphenyltrichloroethane(DDT) and its metabolites in air and precipitation of the Pearl River delta,China[J].Chemosphere,84:446-451
Zhang L,Lohmann R.2010.Cycling of PCBs and HCB in the surface ocean-lower atmosphere of the open Pacific[J].Environmental Science & Technology,44:3832-3838
Bruhn R,Lakaschus S,McLachlan M S.2003.Air/sea gas exchange of PCBs in the southern Baltic Sea[J].Atmos Environ,37(24):3445-3454
Caro L,Mai N,Heinrich H,et al.2016.Theobald persistent organochlorine pesticides and polychlorinated biphenyls in air of the North Sea region and air-sea exchange[J].Environmental Science and Pollution Research,23:23648-23661
Castro-Jiménez J,Mariani G,Vives I,et al.2011.Atmospheric concentrations,occurrence and deposition of persistent organic pollutants (POPs) in a Mediterranean coastal site (Etang de Thau,France)[J].Environmental Pollution,159(7):1948-1956
Duce R A,Liss P S,Merrill J T,et al.1998.The atmosphere input of trace species to the world ocean[J].Global Biogeochemical Cycles,5(3):193-259
Fu X W,Yang X,Tan Q Y,et al.22018.Isotopic composition of gaseous elemental mercury in the marine boundary layer of East China Sea[J].Atmospheres,123(14):7656-7669
Gevao B J,Hamilton-Taylor J,Jones K C,et al.1998.Polychlorinated biphenyl and polycyclic aromatic hydrocarbon deposition to and exchange at the air-water interface of Esthwaite Water,a small lake in Cumbria,UK[J].Environmental Pollution,102(1):63-75
Günindi M,Tasdemir Y.2010.Atmospheric polychlorinated biphenyl (PCB) inputs to a coastal city near the marmara sea [J].Marine Pollution Bulletin,60(12):2242-2250
Günindi M,Tasdemir Y.2011.Wet and dry deposition fluxes of polychlorinated biphenyls (PCBs) in an urban area of Turkey[J].Water,Air,& Soil Pollution,215(1/4):427-439
Jaward F,Barber J L,Booij K,et al.2004.Evidence for dynamic air-water coupling and cycling of persistent organic pollutants over the open Atlantic Ocean[J].Environmental Science and Technology,38(9):2617-2625
Jiang Y Q,Lin T,Wu Z L,et al.2018.Seasonal atmospheric deposition and air-sea gas exchange of polycyclic aromatic hydrocarbons over the Yangtze River Estuary,East China Sea:Implications for source-sink processes[J].Atmospheric Environment,178:31-40
Lammel G,Audy O,Besis A,et al.2015.Air and seawater pollution and air-sea gas exchange of persistent toxic substances in the Aegean Sea:spatial trends of PAHs,PCBs,OCPs and PBDEs[J].Environmental Science and Pollution Research,22(15):11301-11313
Lao Q B,Jiao L P,Chen F J,et al.2018.Influential factors and dry deposition of polychlorinated biphenyls (PCBs) in atmospheric particles at an isolated island (Ping tan Island) in Fujian Province,China[J].Atmosphere,9(2):59
Lee W J,Su C C,Shen H,et al.1996.Monitoring and modeling of PCB dry deposition in urban area [J].Hazard.Mater,49:57-88
李英明,江桂斌,王亚韡,等.2008.电子垃圾拆解地大气中二恶英、多氯联苯、多溴联苯醚的污染水平及相分配规律[J].科学通报,53(2):165-171
Li Z X,Lin T,Li Y Y,et al.2016.Atmospheric deposition and air-sea gas exchange fluxes of DDT and HCH in the Yangtze River Estuary,East China Sea[J].Atmosphere,122:7664-7677
Lisa A T,Cari L G,Daryl A V,et al.2004.Atmospheric concentrations and deposition of polychorinated biphenyls to the Hudson River Estuary[J].Environ Sci Technol,38 (9):2568-2573
Lisa A T,Maya P,Steven J E,et al.2006.Direct and indirect atmospheric deposition of PCBs to the Delaware River Watershed [J].Environ Sci Technol,40 (7):2171-2176
Manchester-Neesving J B,Andren A W.1989.Seasonal variation in the atmosphere concentration of polychlorinated biphenyls congeners[J].Environmental Science and Technology,23(9):1138-1148
Mandalakis M,Staphanou E G.2002.Study of atmospheric PCB concentrations over the eastern Mediterranean Sea [J].Journal of Geophysical Research:Atmospheres,107(23):4716- 4729
Manolis M K,Euripides G S.2004.Wet Deposition of polychlorinated biphenyls in the Eastern Mediterranean[J].Environ Sci Technol,38:3011-3018
Mi H H,Wu Z S,Lin L F,et al.2012.Atmospheric dry deposition of polychlorinated dibenzo-p-dioxins/dibenzofurans (PCDD/Fs) and polychlorinated biphenyls(PCBs) in Southern Taiwan[J].Aerosol and Air Quality Research,12:1016-1029
Montone R C,Taniguchi S,Boian C,et al.2005.PCBs and chlorinated pesticides(DDTs,HCHs and HCB) in the atmosphere of the southwest Atlantic and Antarctic oceans[J].Mar Pollut Bull Baseline,50(7):778-786
Montone R C,Taniguchi S,Weber R R,et al.2003.PCBs in the atmosphere of King George Island,Antarctica[J].Science of the Total Environment,308(1/3):167-173
Mustafa O,Banu C,Eylem D,et al.2008.Air-water exchange of polychlorinated biphenyls (PCBs) and organochlorine pesticides (OCPs) at a coastal site in Izmir Bay,Turkey[J].Marine Chemistry,109(1/2):115-129
Odabasi M,Cetin B,Demircioglu E,et al.2008.Air-water exchange of polychlorinated biphenyls (PCBs) and organochlorine pesticides (OCPs) at a coastal site in Izmir Bay,Turkey[J].Marine Chemistry,109(1/2):115-129
Simcik M F,Basu I,Sweet C W,et al.1999.Temperature dependence and temporal trends of polychlorinated biphenyl congener in the Great Lakes atmosphere[J].Environmental Science and Technology,33(12):1991-1995
Simcik M F,Zhang H,Eisenreich S J,et al.1997.Urban contamination of the Chicago/Coastal Lake Michigan atmosphere by PCBs and PAHs during AEOLOS[J].Environmental Science and Technology,31(7):2141-2147
王飞,2015.持久性有机污染物多氯联苯(PCBs)的研究进展[J].科技资讯,(20):139-143
Wania F,Haugen J E,Lei Y D,et al.1998.Temperature dependence of atmospheric concentrations of semivolatile organic compounds[J].Environmental Science & Technology,32:1013-1021
杨国胜,马玲玲,许殿斗,等,2012.北京市石景山区夏季雨水和大气中PCBs的特征解析[J].中国环境科学,32(7):1234-1240
Yue Q,Zhang K,Zhang B Z,et al.2011.Occurrence,phase distribution and depositional intensity of dichlorodiphenyltrichloroethane(DDT) and its metabolites in air and precipitation of the Pearl River delta,China[J].Chemosphere,84:446-451
Zhang L,Lohmann R.2010.Cycling of PCBs and HCB in the surface ocean-lower atmosphere of the open Pacific[J].Environmental Science & Technology,44:3832-3838