博斯腾湖流域大气多环芳烃污染特征、干沉降通量及来源
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摘要
本研究使用大气被动采样器(PAS-PUF)和干沉降被动采样器(PAS-DD),分别于2016年采暖期和2017年非采暖期对新疆博斯腾湖流域及周边地区15种USEPA优控多环芳烃(PAHs)大气浓度和干沉降进行了观测,并对其污染特征和来源进行了研究.结果表明,采暖期和非采暖期博斯腾湖流域PAHs大气浓度范围分别为6. 38～245. 43 ng·m~(-3)和2. 33～74. 76ng·m~(-3);采暖期与非采暖期均呈现出居民区>湖泊周边>塔中的空间分布.采暖期和非采暖期PAHs大气干沉降通量范围分别为0. 45～18. 10μg·(m~2·d)-1和0. 25～8. 15μg·(m~2·d)-1;采暖期居民区PAHs干沉降通量比湖泊周边和塔中采样点高,但在非采暖期塔中采样点高于其它采样点.整体而言,博斯腾湖流域大气及干沉降中PAHs在采暖期显著高于非采暖期,在采暖期与非采暖期均以菲(Phe)、芴(Flu)、荧蒽(Flua)和芘(Pyr)等3～4环PAHs为主.比值法源解析结果显示,博斯腾湖流域大气和干沉降中PAHs主要来源于煤炭和生物质燃烧; HYSPLIT前向和后向轨迹模拟结果表明,非采暖期居民区较高PAHs排放通过大气传输到达博斯腾湖区,经大气干沉降进入水体,可能会对博斯腾湖水生环境造成影响.
Passive air samplers( PAS-PUF) and passive dry deposition( PAS-DD) samplers were applied in the Bosten Lake watershed located in Xinjiang to estimate the atmospheric concentrations and dry deposition fluxes for 15 US EPA priority polycyclic aromatic hydrocarbons( PAHs) during a heating period in 2016 and no-heating period in 2017,respectively. The results showed that the atmospheric PAHs concentrations in the Bosten oasis area ranged from 6. 38 ng·m~(-3) to 245. 43 ng·m~(-3) during the heating period and 2. 33 ng·m~(-3) to 74. 76 ng·m~(-3) during the non-heating period. The highest atmospheric PAHs concentrations were found in the residential area,followed by regions near Bosten Lake and Tazhong. The atmospheric dry deposition fluxes of PAHs in the Bosten Lake watershed ranged from 0. 45 μg·( m~2·d)-1 to 18. 10 μg·( m~2·d)-1 during the heating period and 0. 25 μg·( m~2·d)-1 to 8. 15μg·( m~2·d)-1 during the non-heating period. During the heating period,the atmospheric dry deposition fluxes in the residential area were significantly higher than those in the regions near Bosten Lake and Tazhong. However,the atmospheric PAHs dry deposition flux in Tazhong was much higher than that in other sites during the heating and no-heating periods. In general,the atmospheric PAHs dry deposition fluxes during the heating period were significantly higher than those during the non-heating period. PAH composition for the atmosphere and dry deposition were dominated by 3 and 4 ring congeners,especially by phenanthrene,fluorine,fluoranthene,and pyrene during two sampling periods. In addition,the congener diagnostic ratio shows that coal and biomass combustion were possible sources of atmospheric PAHs in the Bosten Lake watershed. The forward and backward trajectory analysis based on the HYSPLIT model demonstrated that the higher atmospheric PAH emissions from the residential area would be transported to Bosten Lake,which can affect the aquatic environment of this lake by dry deposition.
Passive air samplers( PAS-PUF) and passive dry deposition( PAS-DD) samplers were applied in the Bosten Lake watershed located in Xinjiang to estimate the atmospheric concentrations and dry deposition fluxes for 15 US EPA priority polycyclic aromatic hydrocarbons( PAHs) during a heating period in 2016 and no-heating period in 2017,respectively. The results showed that the atmospheric PAHs concentrations in the Bosten oasis area ranged from 6. 38 ng·m~(-3) to 245. 43 ng·m~(-3) during the heating period and 2. 33 ng·m~(-3) to 74. 76 ng·m~(-3) during the non-heating period. The highest atmospheric PAHs concentrations were found in the residential area,followed by regions near Bosten Lake and Tazhong. The atmospheric dry deposition fluxes of PAHs in the Bosten Lake watershed ranged from 0. 45 μg·( m~2·d)-1 to 18. 10 μg·( m~2·d)-1 during the heating period and 0. 25 μg·( m~2·d)-1 to 8. 15μg·( m~2·d)-1 during the non-heating period. During the heating period,the atmospheric dry deposition fluxes in the residential area were significantly higher than those in the regions near Bosten Lake and Tazhong. However,the atmospheric PAHs dry deposition flux in Tazhong was much higher than that in other sites during the heating and no-heating periods. In general,the atmospheric PAHs dry deposition fluxes during the heating period were significantly higher than those during the non-heating period. PAH composition for the atmosphere and dry deposition were dominated by 3 and 4 ring congeners,especially by phenanthrene,fluorine,fluoranthene,and pyrene during two sampling periods. In addition,the congener diagnostic ratio shows that coal and biomass combustion were possible sources of atmospheric PAHs in the Bosten Lake watershed. The forward and backward trajectory analysis based on the HYSPLIT model demonstrated that the higher atmospheric PAH emissions from the residential area would be transported to Bosten Lake,which can affect the aquatic environment of this lake by dry deposition.
引文
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[14]王慧琴.塔里木盆地TSP中碳质气溶胶和多环芳烃污染特征与来源分析及数值模拟[D].兰州:兰州大学,2016.
[15]杨振,雷军,段祖亮,等.新疆人口的空间分布特征[J].地理研究,2016,35(12):2333-2346.Yang Z, Lei J, Duan Z L, et al. Spatial distribution of population in Xinjiang[J]. Geographical Research,2016,35(12):2333-2346.
[16]沈贝贝,吴敬禄,赵中华,等.新疆开都河流域不同环境介质中的有机氯农药和多环芳烃残留及分布特征[J].矿物岩石地球化学通报,2016,35(4):646-652.Shen B B,Wu J L,Zhao Z H,et al. Residue and distribution characteristics of organochlorine pesticides and polycyclic aromatic hydrocarbons in different environmental components of the Kaidu River Catchment, Xinjiang[J]. Bulletin of Mineralogy,Petrology and Geochemistry,2016,35(4):646-652.
[17] Ma W L,Liu L Y,Jia H L,et al. PAHs in Chinese atmosphere part I:concentration,source and temperature dependence[J].Atmospheric Environment,2018,173:330-337.
[18]吾拉尔·哈那哈提,迪丽努尔·塔力甫,买里克扎提·买合木提,等.乌鲁木齐市大气可吸入颗粒物中多环芳烃的污染特征及来源解析[J].环境污染与防治,2015,37(1):35-40.Wulaer H, Dilinuer T, Mailikezati M, et al. Source apportionment of atmospheric polycyclic aromatic hydrocarbons in inhalable particulate matter at heating and non-heating periods in Urumqi,China[J]. Environmental Pollution and Control,2015,37(1):35-40.
[19] Wang L,Zhao Y,Yi X,et al. Spatial distribution of atmospheric PAHs and their genotoxicity in petrochemical industrialized Lanzhou valley,Northwest China[J]. Environmental Science and Pollution Research,2017,24(14):12820-12834.
[20] Ma W L,Li Y F,Qi H,et al. Seasonal variations of sources of polycyclic aromatic hydrocarbons(PAHs)to a northeastern urban city,China[J]. Chemosphere,2010,79(4):441-447.
[21]阚海东.《环境空气质量标准》(GB3095-2012)细颗粒物(PM2. 5)标准值解读[J].中华预防医学杂志,2012,46(5):396-398.
[22]吴甜,王晓龙,刘子龙,等.石河子市大气总悬浮颗粒物的浓度和其中多环芳烃的分析[J].石河子大学学报(自然科学版),2015,33(5):604-609.Wu T,Wang X L,Liu Z L,et al. Study on the concentration and polycyclic aromatic hydrocarbons compentents of total suspended particles in Shihezi[J]. Journal of Shihezi University(Natural Science),2015,33(5):604-609.
[23] Harner T,Su K,Genualdi S,et al. Calibration and application of PUF disk passive air samplers for tracking polycyclic aromatic compounds(PACs)[J]. Atmospheric Environment,2013,75:123-128.
[24]马万里,李一凡,孙德智,等.哈尔滨市大气气相中多环芳烃的研究[J].环境科学,2009,30(11):3167-3172.Ma W L,Li Y F,Sun D Z,et al. Gaseous polycyclic aromatic hydrocarbons in Harbin air[J]. Environmental Science,2009,30(11):3167-3172.
[25]张利飞,杨文龙,董亮,等.利用PUF被动采样技术研究长三角城市群大气中多环芳烃的时空分布及来源[J].环境科学,2013,34(9):3339-3346.Zhang L F,Yang W L,Dong L,et al. PUF passive air sampling of polycyclic aromatic hydrocarbons in atmosphere of the Yangtze River Delta,China:spatio-temporal distribution and potential sources[J]. Environmental Science,2013,34(9):3339-3346.
[26]张腾林,迪丽努尔·塔力甫,王新明,等.乌鲁木齐市典型城区大气PAHs气-粒分配特征[J].环境科学研究,2016,29(10):1408-1416.Zhang T L,Dilnur T,Wang X M,et al. Gas-particle partitioning of atmospheric polycyclic aromatic hydrocarbons in the urban area of Urumqi City,China[J]. Research of Environmental Sciences,2016,29(10):1408-1416.
[27] Pokhrel B,Gong P,Wang X P,et al. Polycyclic aromatic hydrocarbons in the urban atmosphere of Nepal:distribution,sources,seasonal trends,and cancer risk[J]. Science of the Total Environment,2017,618:1583-1590.
[28]lvarezáL,Pozo K,Paéz M I,et al. Semivolatile Organic Compounds(SVOCs)in the atmosphere of Santiago de Cali,Valle del Cauca, Colombia along north-south transect using polyurethane foam disk as passive air samplers[J]. Atmospheric Pollution Research,2016,7(6):945-953.
[29] Evci Y M,Esen F,Ta爧demir Y. Monitoring of long-term outdoor concentrations of PAHs with passive air samplers and comparison with meteorological data[J]. Archives of Environmental Contamination and Toxicology,2016,71(2):246-256.
[30]刘强吉,武胜利.新疆博斯腾湖流域最高气温趋势分析[J].安徽农业科学,2015,43(27):178-180.Liu Q J,Wu S L. Trends analysis for maximum temperature in the Bosten Lake Basin of Xinjiang[J]. Journal of Anhui Agricultural Sciences,2015,43(27):178-180.
[31] He Q S,Zhang L,Cui Y,et al. Particle dry deposition of polycyclic aromatic hydrocarbons and its risk assessment in a typical coal-polluted and basin city, Northern China[J].Atmospheric Pollution Research,2017,8(6):1081-1089.
[32] 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.
[33]王戎,郎畅,曹军,等.基于轨迹计算的污染物归趋概率模型[J].环境科学学报,2009,29(8):1598-1603.Wang R, Lang C, Cao J, et al. A probabilistic model for transport of air pollutants based on forward trajectory calculations[J]. Acta Scientiae Circumstantiae,2009,29(8):1598-1603.
[2] Laflamme R E,Hites R A. The global distribution of polycyclic aromatic hydrocarbons in recent sediments[J]. Geochimica et Cosmochimica Acta,1988,42(3):289-303.
[3] Ravindra K,Sokhi R,Van Grieken R. Atmospheric polycyclic aromatic hydrocarbons:source attribution,emission factors and regulation[J]. Atmospheric Environment,2008,42(13):2895-2921.
[4] Khairy M A, Lohmann R. Source apportionment and risk assessment of polycyclic aromatic hydrocarbons in the atmospheric environment of Alexandria,Egypt[J]. Chemosphere,2013,91(7):895-903.
[5]张华艳.近2. 5ka来博斯腾湖流域环境演变与人类文明的关系研究[D].乌鲁木齐:新疆师范大学,2015.
[6] Lei X N,Li W W,Lu J J,et al. Distribution of polycyclic aromatic hydrocarbons in snow of Mount Nanshan,Xinjiang[J].Water and Environment Journal,2015,29(2):252-258.
[7]沈贝贝,吴敬禄,赵中华,等.近百年来新疆博斯腾湖多环芳烃的组成及变化特征[J].环境科学,2016,37(2):507-512.Shen B B,Wu J L,Zhao Z H,et al. Over one hundred year sediment record of polycyclic aromatic hydrocarbons in the Lake Bosten,Xinjiang[J]. Environmental Science,2016,37(2):507-512.
[8]刘咸德,郑晓燕,王宝盛,等.持久性有机污染物被动采样与区域大气传输[M].北京:科学出版社,2015. 41-55.
[9]张干,刘向.大气持久性有机污染物(POPs)被动采样[J].化学进展,2009,21(2-3):297-306.Zhang G,Liu X. Passive atmospheric sampling of persistent organic pollutants(POPs)[J]. Progress in Chemistry,2009,21(2-3):297-306.
[10] Shoeib M,Harner T. Characterization and comparison of three passive air samplers for persistent organic pollutants[J].Environmental Science&Technology,2002,36(19):4142-4151.
[11] Eng A,Harner T,Pozo K. A prototype passive air sampler for measuring dry deposition of polycyclic aromatic hydrocarbons[J]. Environmental Science&Technology Letters,2014,1(1):77-81.
[12] Wilford B H,Shoeib M,Harner T,et al. Polybrominated diphenyl ethers in indoor dust in Ottawa,Canada:implications for sources and exposure[J]. Environmental Science&Technology,2005,39(18):7027-7035.
[13] Zhang J W,Zhao J,Cai J,et al. Spatial distribution and source apportionment of atmospheric polycyclic aromatic hydrocarbons in the Pearl River Delta, China[J]. Atmospheric Pollution Research,2018,9(5):887-893.
[14]王慧琴.塔里木盆地TSP中碳质气溶胶和多环芳烃污染特征与来源分析及数值模拟[D].兰州:兰州大学,2016.
[15]杨振,雷军,段祖亮,等.新疆人口的空间分布特征[J].地理研究,2016,35(12):2333-2346.Yang Z, Lei J, Duan Z L, et al. Spatial distribution of population in Xinjiang[J]. Geographical Research,2016,35(12):2333-2346.
[16]沈贝贝,吴敬禄,赵中华,等.新疆开都河流域不同环境介质中的有机氯农药和多环芳烃残留及分布特征[J].矿物岩石地球化学通报,2016,35(4):646-652.Shen B B,Wu J L,Zhao Z H,et al. Residue and distribution characteristics of organochlorine pesticides and polycyclic aromatic hydrocarbons in different environmental components of the Kaidu River Catchment, Xinjiang[J]. Bulletin of Mineralogy,Petrology and Geochemistry,2016,35(4):646-652.
[17] Ma W L,Liu L Y,Jia H L,et al. PAHs in Chinese atmosphere part I:concentration,source and temperature dependence[J].Atmospheric Environment,2018,173:330-337.
[18]吾拉尔·哈那哈提,迪丽努尔·塔力甫,买里克扎提·买合木提,等.乌鲁木齐市大气可吸入颗粒物中多环芳烃的污染特征及来源解析[J].环境污染与防治,2015,37(1):35-40.Wulaer H, Dilinuer T, Mailikezati M, et al. Source apportionment of atmospheric polycyclic aromatic hydrocarbons in inhalable particulate matter at heating and non-heating periods in Urumqi,China[J]. Environmental Pollution and Control,2015,37(1):35-40.
[19] Wang L,Zhao Y,Yi X,et al. Spatial distribution of atmospheric PAHs and their genotoxicity in petrochemical industrialized Lanzhou valley,Northwest China[J]. Environmental Science and Pollution Research,2017,24(14):12820-12834.
[20] Ma W L,Li Y F,Qi H,et al. Seasonal variations of sources of polycyclic aromatic hydrocarbons(PAHs)to a northeastern urban city,China[J]. Chemosphere,2010,79(4):441-447.
[21]阚海东.《环境空气质量标准》(GB3095-2012)细颗粒物(PM2. 5)标准值解读[J].中华预防医学杂志,2012,46(5):396-398.
[22]吴甜,王晓龙,刘子龙,等.石河子市大气总悬浮颗粒物的浓度和其中多环芳烃的分析[J].石河子大学学报(自然科学版),2015,33(5):604-609.Wu T,Wang X L,Liu Z L,et al. Study on the concentration and polycyclic aromatic hydrocarbons compentents of total suspended particles in Shihezi[J]. Journal of Shihezi University(Natural Science),2015,33(5):604-609.
[23] Harner T,Su K,Genualdi S,et al. Calibration and application of PUF disk passive air samplers for tracking polycyclic aromatic compounds(PACs)[J]. Atmospheric Environment,2013,75:123-128.
[24]马万里,李一凡,孙德智,等.哈尔滨市大气气相中多环芳烃的研究[J].环境科学,2009,30(11):3167-3172.Ma W L,Li Y F,Sun D Z,et al. Gaseous polycyclic aromatic hydrocarbons in Harbin air[J]. Environmental Science,2009,30(11):3167-3172.
[25]张利飞,杨文龙,董亮,等.利用PUF被动采样技术研究长三角城市群大气中多环芳烃的时空分布及来源[J].环境科学,2013,34(9):3339-3346.Zhang L F,Yang W L,Dong L,et al. PUF passive air sampling of polycyclic aromatic hydrocarbons in atmosphere of the Yangtze River Delta,China:spatio-temporal distribution and potential sources[J]. Environmental Science,2013,34(9):3339-3346.
[26]张腾林,迪丽努尔·塔力甫,王新明,等.乌鲁木齐市典型城区大气PAHs气-粒分配特征[J].环境科学研究,2016,29(10):1408-1416.Zhang T L,Dilnur T,Wang X M,et al. Gas-particle partitioning of atmospheric polycyclic aromatic hydrocarbons in the urban area of Urumqi City,China[J]. Research of Environmental Sciences,2016,29(10):1408-1416.
[27] Pokhrel B,Gong P,Wang X P,et al. Polycyclic aromatic hydrocarbons in the urban atmosphere of Nepal:distribution,sources,seasonal trends,and cancer risk[J]. Science of the Total Environment,2017,618:1583-1590.
[28]lvarezáL,Pozo K,Paéz M I,et al. Semivolatile Organic Compounds(SVOCs)in the atmosphere of Santiago de Cali,Valle del Cauca, Colombia along north-south transect using polyurethane foam disk as passive air samplers[J]. Atmospheric Pollution Research,2016,7(6):945-953.
[29] Evci Y M,Esen F,Ta爧demir Y. Monitoring of long-term outdoor concentrations of PAHs with passive air samplers and comparison with meteorological data[J]. Archives of Environmental Contamination and Toxicology,2016,71(2):246-256.
[30]刘强吉,武胜利.新疆博斯腾湖流域最高气温趋势分析[J].安徽农业科学,2015,43(27):178-180.Liu Q J,Wu S L. Trends analysis for maximum temperature in the Bosten Lake Basin of Xinjiang[J]. Journal of Anhui Agricultural Sciences,2015,43(27):178-180.
[31] He Q S,Zhang L,Cui Y,et al. Particle dry deposition of polycyclic aromatic hydrocarbons and its risk assessment in a typical coal-polluted and basin city, Northern China[J].Atmospheric Pollution Research,2017,8(6):1081-1089.
[32] 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.
[33]王戎,郎畅,曹军,等.基于轨迹计算的污染物归趋概率模型[J].环境科学学报,2009,29(8):1598-1603.Wang R, Lang C, Cao J, et al. A probabilistic model for transport of air pollutants based on forward trajectory calculations[J]. Acta Scientiae Circumstantiae,2009,29(8):1598-1603.
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