Atmospheric concentration characteristics and gas/particle partitioning of PCBs from the North Pacific to the Arctic Ocean
-
摘要: 对2012年7月至9月间采集自北太平洋和北冰洋大气中典型多氯联苯(PCBs)的浓度分布与气固分配行为进行了研究.大气中26种PCBs同族物的浓度(∑PCBs) (气相加颗粒相)为19.116 pg/m3,标准偏差为13.833 pg/m3.浓度最高的3种同族物为CB-28,-52和-77,占∑PCBs的43.0%.气相PCBs占∑PCBs的79.0%.本研究观测到∑PCBs与纬度间以及绝对温度倒数(1/T)间的显著负相关关系,同时,对大多数PCBs同族物,也观测到了气固分配系数的对数值(logKP)与1/T间的显著相关关系.PCBs的logKP与其过冷液体饱和蒸汽压(logp°L)具有显著的线性关系,其斜率较小(-0.15至-0.46,均值-0.27),且各样品间的斜率与截距值差别不显著(p > 0.1),表明PCBs在各样品中的吸附/吸收特征和颗粒物组成相似.大气颗粒物中炭黑的存在对分配的影响进行了考察,结果表明黑灰-空气模型的模拟结果要优于传统的J-P模型和基于正辛醇-空其分配系数的模型.分析结果还表明,PCBs在颗粒物元素碳上的吸附作用要强于在颗粒物有机质中的吸收作用,特别是对低氯取代PCBs,该趋势更加显著.Abstract: Polychlorinated biphenyls (PCBs) were measured in atmospheric samples collected from the North Pacific to the Arctic Ocean between July and September 2012 to study the atmospheric concentration characteristics of PCBs and their gas/particle partitioning. The mean concentration of 26 PCBs (vapor plus particulate phase) (∑PCBs) was 19.116 pg/m3 with a standard deviation of 13.833 pg/m3. Three most abundant congeners were CB-28, -52 and -77, accounting for 43.0% to ∑PCBs. The predominance of vapor PCBs (79.0% to ∑PCBs) in the atmosphere was observed. ∑PCBs were negative correlated with the latitudes and inverse of the absolute temperature (1/T). The significant correlation for most congeners was also observed between the logarithm of gas/particle partition coefficient (logKP) and 1/T. Shallower slopes (from -0.15 to -0.46, average -0.27) were measured from the regression of the logarithm of sub-cooled liquid vapor pressures (logp°L) and logKP for all samples. The difference of the slopes and intercepts among samples was insignificant (p>0.1), implying adsorption and/or absorption processes and the aerosol composition did not differ significantly among different samples. By comparing three models, the J-P adsorption model, the octanol/ air partition coefficient (KOA) based model and the soot-air model, the gas/particle partitioning of PCBs in the Arctic atmosphere was simulated more precisely by the soot-air model, and the adsorption onto elemental carbon is more sensitive than the absorption into organic matters of aerosols, especially for lowchlorinated PCB congeners.
-
Key words:
- PCBs /
- gas/particle partitioning /
- Arctic Ocean /
- soot-air model /
- semi-volatile organic compounds
-
Baek S Y, Choi S D, Chang Y S. 2011. Three-year atmospheric monitoring of organochlorine pesticides and polychlorinated biphenyls in Polar Regions and the South Pacific. Environ Sci Technol, 45(10): 4475-4482 Bogdal C, Scheringer M, Abad E, et al. 2012. Worldwide distribution of persistent organic pollutants in air, including results of air monitoring by passive air sampling in five continents. Trend AnalChem, 46: 150-161 Breivik K, Sweetman A, Pacyna J M, et al. 2002. Towards a global historical emission inventory for selected PCB congeners-a mass balance approach: 2. Emissions. Sci Total Environ, 290(1-3): 199-224 Bucheli T D, Gustafsson Ö. 2000. Quantification of the soot-water distribution coefficient of PAHs provides mechanistic basis for enhanced sorption observations. Environ Sci Technol, 34(24): 5144-5151 Callén M S, Cruz M T, López J M, et al. 2008. Some inferences on the mechanism of atmospheric gas/particle partitioning of polycyclic aromatic hydrocarbons (PAHs) at Zaragoza (Spain). Chemo-sphere, 73(8): 1357-1365 Dachs J, Eisenreich S J. 2000. Adsorption onto aerosol soot carbon dominates gas-particle partitioning of polycyclic aromatic hydrocarbons.Environ Sci Technol, 34(17): 3690-3697 Finzio A, Mackay D, Bidleman T F, et al. 1997. Octanol-air partition coefficient as a predictor of partitioning of semivolatile organic chemicals to aerosols. Atmos Environ, 31(15): 2289-2296 Gaga E O, Ari A. 2011. Gas-particle partitioning of polycyclic aromatic hydrocarbons (PAHs) in an urban traffic site in Eskisehir, Turkey.Atmos Environ, 99(2): 207-216 Galbán-Malagón C J, Vento S D, Cabrerizo A, et al. 2013. Factors affecting the atmospheric occurrence and deposition of polychlorinated biphenyls in the Southern Ocean. Atmos Chem Phys, 13(23): 12029-12041 Gambaro A, Manodori L, Zangrando R, et al. 2005. Atmospheric PCB concentrations at Terra Nova bay, Antarctica. Environ Sci Technol, 39(24): 9406-9411 Harner T, Bidleman T F. 1998. Octanol-air partition coefficient for describing particle/gas partitioning of aromatic compounds in urban air. Environ Sci Technol, 32(10): 1494-1502 He J, Balasubramanian R. 2009. A study of gas/particle partitioning ofSVOCs in the tropical atmosphere of Southeast Asia. Atmos Environ, 43(29): 4375-4383 Helma P A, Bidleman T F. 2005. Gas-particle partitioning of polychlorinated naphthalenes and non-and mono-ortho-substituted polychlorinated biphenyls in arctic air. Sci Total Environ, 342(1- 3): 161-173 Hung H, Halsall C J, Blanchard P, et al. 2001. Are PCBs in the CanadianArctic atmosphere declining? Evidence from 5 years of monitoring.Environ Sci Technol, 35(7): 1303-1311 Junge C E. 1977. Fate of pollutants in the air and water environments.In: Suffet I H, ed. New York: Wiley-Interscience, 7-26 Kaupp H, McLachlan M S. 1999. Gas/particle partitioning of PCDD/Fs,PCBs, PCNs and PAHs. Chemosphere, 38(14): 3411-3421 Li Xuehua, Chen Jingwen, Zhang Li, et al. 2006. The fragment constant method for predicting octanol-air partition coefficients of persistent organic pollutants at different temperatures. J Phys ChemRef Data, 35(3): 1365-1384 Lohmann R, Lammel G. 2004. Adsorptive and absorptive contributions to the gas-particle partitioning of polycyclic aromatic hydrocarbons: state of knowledge and recommended parameterization for modeling. Environ Sci Technol, 38(14): 3793-3801 Ma J, Hung H, Tian C, et al. 2011. Revolatilization of persistent organic pollutants in the Arctic induced by climate change. Nature ClimateChange, 1(5): 255-260 Mandalakis M, Stephanou E G. 2002. Study of atmospheric PCB concentrations over the eastern Mediterranean Sea. J Geophys Res, 107(D23): ACH 18-1-ACH 18-14 Mandalakis M, Stephanou E G. 2007. Atmospheric concentration characteristics and gas/particle partitioning of PCBs in a rural area ofEastern Germany. Environ Pollut, 147(1): 211-221 Montone R C, Taniguchi S, Weber R R. 2003. PCBs in the atmosphere of King George Island, Antarctica. Sci Total Environ, 308(1-3): 167-173 Newton S R, Bidleman T, Bergknut M, et al. 2013. Atmospheric deposition of persistent organic pollutants and chemicals of emerging concern at two sites in northern Sweden. Environ Sci: ProcessesImpacts, 15(2): 298-305 Odabasi M, Cetin E, Sofuoglu A. 2006. Determination of octanol-air partition coefficients and supercooled liquid vapor pressures ofPAHs as a function of temperature: application to gas-particle partitioning in an urban atmosphere. Atmos Environ, 40(34): 6615-6625 Pankow J F. 1987. Review and comparative analysis of the theories on partitioning between the gas and aerosol particulate phases in the atmosphere. Atmos Environ, 21(11): 2275-2283 Pankow J F. 1994. Absorption model of the gas/aerosol partitioning involved in the formation of secondary organic aerosol. AtmosEnviron, 28(2): 189-193 Pankow J F, Bidleman T F. 1992. Interdependence of the slopes and intercepts from log-log correlations of measured gas-particle partitioning and vapor pressure—I. Theory and analysis of available data. Atmos Environ, 26(6): 1071-1080 Simcik M F, Franz T P, Zhang H, et al. 1998. Gas/particle partitioning of PCBs and PAHs in the Chicago urban and adjacent coastal atmosphere: states of equilibrium. Environ Sci Technol, 32(2): 251-257 Sitaras L E, Bakeas E B, Siskos P A. 2004. Gas/particle partitioning of seven volatile polycyclic aromatic hydrocarbons in a heavy traffic urban area. Sci Total Environ, 327(1-3): 249-264 van Noort P C M. 2003. A thermodynamics-based estimation model for adsorption of organic compounds by carbonaceous materials in environmental sorbents. Environ Toxicol Chem, 22(6): 1179-1188 van Noort P C M. 2009. QSPRs for the estimation of subcooled liquid vapor pressures of polycyclic aromatic hydrocarbons, and of polychlorinated benzenes, biphenyls, dibenzo-p-dioxins, and dibenzofurans at environmentally relevant temperatures. Chemosphere, 77(6): 848-853 Vardar N, Esen F, Tasdemir Y. 2008. Seasonal concentrations and partitioning of PAHs in a suburban site of Bursa, Turkey. Environ Pollut, 155(2): 298-307 Wang Zhen, Na Guangshui, Ma Xindong, et al. 2013. Occurrence and gas/particle partitioning of PAHs in the atmosphere from theNorth Pacific to the Arctic Ocean. Atmos Environ, 77: 640-646 Wang Zhen, Ren Peifang, Sun Yan, et al. 2013. Gas/particle partitioning of polycyclic aromatic hydrocarbons in coastal atmosphere of the north Yellow Sea, China. Environ Sci Pollut Res, 20(8): 5753-5763 Wania F, Haugen J E, Lei Y D, et al. 1998. Temperature dependence of atmospheric concentrations of semivolatile organic compounds.Environ Sci Technol, 32(8): 1013-1021 Yamasaki H, Kuwata K, Miyamoto H. 1982. Effect of ambient temperature on aspects of airborne polycyclic aromatic hydrocarbons.Environ Sci Technol, 16(4): 189-194
点击查看大图
计量
- 文章访问数: 1374
- HTML全文浏览量: 22
- PDF下载量: 1867
- 被引次数: 0