昆明松华坝水库沉积物中PAHs垂直分布特征及其来源
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摘要
为揭示昆明松华坝水库人类活动对PAHs(多环芳烃)的影响程度及其污染历史,研究了松华坝水库2根沉积柱(包括集水区人口较密集的1号柱和以山地为主的2号柱)中16种PAHs的垂直分布特征及其来源.结果表明:1号、2号柱中∑16PAHs(16种PAHs总量)分布范围分别为155. 9～471. 3和100. 7～316. 3 ng/g,但1号柱污染程度高于2号柱,可能与其集水区较高的人为排放有关. 1号柱中∑16PAHs整体随采样深度的下降而降低,2号柱则随采样深度的下降而增长;这2根柱子PAHs的组成相似,沉积物中PAHs均以2环的Nap(萘)和3环的Phe(菲)为主(二者占比高于50%),高致癌性的4～6环PAHs也有较大占比.分子比值法和正定矩阵因子分解法结果显示,1号柱中PAHs主要来源顺序为生物质燃烧源(38. 8%)>石油源(34. 7%)>煤炭燃烧源(13. 4%)>石化燃料燃烧源(13. 1%),2号柱主要来源为石油源(44. 4%)>生物质燃烧源(26. 2%)>煤炭燃烧源(15. 3%)>石化燃料燃烧源(14. 1%),反映了集水区人类活动方式与强度对沉积物中PAHs的控制作用.
In order to reveal the influence of human activities on the pollution of PAHs in the Songhuaba Reservoir in Kunming City,Yunnan Province,the vertical distribution and sources of PAHs in the two sedimentary core samples collected from the reservoir were studied. Core 1 was collected from the densely populated catchment area,while the catchment of Core 2 was collected from mountain watershed. The results show that the contents of ∑16 PAHs in Cores 1 and 2 ranged from 155. 9 to 471. 3 ng/g,and from 100. 7 to 316. 3 ng/g,respectively. The pollution level of Core 1 was higher than that of Core 2,which might be related to the higher anthropogenic emissions in the former area. The contents of ∑16 PAHs increased from the bottom to the top in Core 1 while it exhibited a decreasing trend from bottom up in Core 2. For the composition of PAHs,2-ring Nap and 3-ring Phe accounted for more than 50% of ∑16 PAHs,and 4-6-ring PAHs with high carcinogenicity also had a large proportion. The results of both molecular ratio method and positive definite matrix factorization( positive matrix factorization,PMF) indicated that the main sources of PAHs were biomass fuel combustion( 38. 8%),petroleum( 34. 7%),coal burning( 13. 4%),and fossil fuel combustion( 13. 1%) for Core 1 and petroleum( 44. 4%),biomass fuel combustion( 26. 2%),coal burning( 15. 3%),and fossil fuel burning( 14. 1%) for Core 2,reflecting the differential patterns and intensities of human activities in those catchment areas.
In order to reveal the influence of human activities on the pollution of PAHs in the Songhuaba Reservoir in Kunming City,Yunnan Province,the vertical distribution and sources of PAHs in the two sedimentary core samples collected from the reservoir were studied. Core 1 was collected from the densely populated catchment area,while the catchment of Core 2 was collected from mountain watershed. The results show that the contents of ∑16 PAHs in Cores 1 and 2 ranged from 155. 9 to 471. 3 ng/g,and from 100. 7 to 316. 3 ng/g,respectively. The pollution level of Core 1 was higher than that of Core 2,which might be related to the higher anthropogenic emissions in the former area. The contents of ∑16 PAHs increased from the bottom to the top in Core 1 while it exhibited a decreasing trend from bottom up in Core 2. For the composition of PAHs,2-ring Nap and 3-ring Phe accounted for more than 50% of ∑16 PAHs,and 4-6-ring PAHs with high carcinogenicity also had a large proportion. The results of both molecular ratio method and positive definite matrix factorization( positive matrix factorization,PMF) indicated that the main sources of PAHs were biomass fuel combustion( 38. 8%),petroleum( 34. 7%),coal burning( 13. 4%),and fossil fuel combustion( 13. 1%) for Core 1 and petroleum( 44. 4%),biomass fuel combustion( 26. 2%),coal burning( 15. 3%),and fossil fuel burning( 14. 1%) for Core 2,reflecting the differential patterns and intensities of human activities in those catchment areas.
引文
[1]刘宗峰,郎印海,曹正梅,等.黄河口表层沉积物多环芳烃污染源解析研究[J].环境科学研究,2008,21(5):79-84.LIU Zongfeng,LANG Yinhai,CAO Zhengmei,et al. Source apportionment of PAHs in estuarine sediments from the Yellow River[J].Research of Environmental Sciences,2008,21(5):79-84.
[2] BARAKAT A O,MOSTAFA A,WADE T L,et al. Spatial distribution and temporal trends of polycyclic aromatic hydrocarbons(PAHs)in sediments from Lake Maryut,Alexandria,Egypt[J].Water,Air and Soil Pollution,2011,218:63-80.
[3]李宽,周家斌,袁畅,等.武汉市大气PM2. 5中多环芳烃的分布特征及来源[J].环境科学研究,2018,31(4):648-656.LI Kuan,ZHOU Jiabin,YUAN Chang,et al. Characteristics and source apportionment of polycyclic aromatic hydrocarbons in atmospheric PM2. 5of Wuhan City,China[J]. Research of Environmental Sciences,2018,31(4):648-656.
[4]孙小静,石纯,许世远,等.上海北部郊区土壤多环芳烃含量及来源分析[J].环境科学研究,2008,21(4):140-144.SUN Xiaojing,SHI Chun,XU Shiyuan,et al. Concentration and sources of polycyclic aromatic hydrocarbons in surface soil of north suburban Shanghai,China[J]. Research of Environmental Sciences,2008,21(4):140-144.
[5] MENZIE C A,POTOKI B B,SANTODOMATO J. Exposure to carcinogenic PAHs in the environment[J]. Environmental Science&Technology,1992,26(7):1278-1284.
[6]宁怡,柯用春,邓建才,等.巢湖表层沉积物中多环芳烃分布特征及来源[J].湖泊科学,2012,24(6):891-898.NING Yi,KE Yongchun,DENG Jiancai,et al. Distribution and sources of polycyclic aromatic hydrocarbons(PAHs)in surface sediment in Lake Chaohu[J].Lake Sciences,2012,24(6):891-898.
[7]朱春贤.滇池及其流域的经营管理问题[J].环境科学导刊,2010,29(5):25-28.ZHU Chunxian. Management and administration of Dianchi Basin[J].Environmental Science Survey,2010,29(5):25-28.
[8]李珊英,陶玉强,姚书春,等.我国湖泊沉积物多环芳烃的分布特征及来源分析[J].第四纪研究,2015,35(1):118-130.LI Shanying,TAO Yuqiang,YAO Shuchun,et al. Distribution and sources of polycyclic aromatic hydrocarbons(PAHs)in lake sediments from China[J].Quaternary Sciences,2015,35(1):118-130.
[9]任真臻,付伟.松华坝水库水质变化趋势与防护措施研究[J].环境科学导刊,2017,36(1):18-20.REN Zhenzhen,FU Wei.Trend analysis of water quality and water pollution control of Songhuaba Reservoir[J].Environmental Science Survey,2017,36(1):18-20.
[10]许正雄,夏云红.松华坝水源保护区自然地理要素综合分析[J].云南师范大学学报,1992,12(3):123-128.XU Zhengxiong,XIA Yunhong. Synthesis analysis on natural georaphy's key elements of Song-Hua-Dam source of water proecoion region[J]. Journal of Yunnan Normal University,1992,12(3):123-128.
[11]邬莉,陈静,朱晓东,等.农村秸秆焚烧的原因及对策研究[J].中国人口·资源与环境,2001,11(51):110-112.WU Li,CHEN Jing,ZHU Xiaodong,et al. Straw-burning in rural areas of China:causes and controlling strategy[J]. China Population,Resources and Environment,2001,11(51):110-112.
[12]赵语.松华坝水源区保护研究[D].昆明:云南大学,2015:1-49.
[13]赵中昆.松华坝库区水污染与防治研究[J].云南环境科学,2005,24(3):46-47.ZHAO Zhongkun. Research on controlling water pollution of Songhuaba Reservoir[J].Yunnan Environmental Science,2005,24(3):46-47.
[14]沈成达.松华坝水源保护区应实行以林为主林、农、牧、副结合的产业结构[R].昆明:林业局国家林业局昆明勘察设计院,1990:37-38.
[15]郭建阳,廖海清,韩梅,等.密云水库沉积物中多环芳烃的垂直分布、来源及生态风险评估[J].环境科学,2010,31(3):626-631.GUO Jianyang,LIAO Haiqing,HAN Mei,et al. Temporal distribution,sources,and risk assessment of polycyclic aromatic hydrocarbons in sediment core from Miyun Reservoir[J].Environmental Science,2010,31(3):626-631.
[16]赵健,周怀东,富国,等.河北西大洋水库沉积物中多环芳烃的分布、来源及生态风险评价[J].湖泊科学,2011,23(5):701-707.ZHAO Jian,ZHOU Huaidong,FU Guo,et al. Distributions,sources and ecological risk assessment of polycyclic aromatic hydrocarbons in sediments from Xidayang Reservoir,Hebei Province[J]. Lake Sciences,2011,23(5):701-707.
[17]孙盼盼,谢标,周迪,等.滇池流域宝象河水库沉积物中多环芳烃的垂直分布特征及来源解析[J].环境科学学报,2016,36(10):3615-3622.SUN Panpan,XIE Biao,ZHOU Di,et al. Vertical profile and sources of polycyclic aromatic hydrocarbons in a sediment core from Baoxianghe Reservoir in Dianchi Watershed[J]. Acta Scientiae Circumstantiae,2016,36(10):3615-3622.
[18]李秋华,郭建阳,朱元荣,等.滇池PAHs的沉积记录、来源及其生态风险评估[J].环境科学学报,2013,33(9):2565-2572.LI Qiuhua,GUO Jianyang,ZHU Yuanrong,et al. Sedimentary record,sources and risk assessment of polycyclic aromatic hydrocarbons in Dianchi Lake,southwest China[J]. Acta Scientiae Circumstantiae,2013,33(9):2565-2572.
[19] FERNANDES M B,SICRE M A,BOIREAU A. et al. Polyaromatic hydrocarbon(PAH)distributions in the Seine River and its estuary[J].Marine Pollution Bulletin,1997,34(11):857-867.
[20] KANNAN K,JOHNSON-RESTREPO B,YOHN S S,et al. Spatial and temporal distribution of polycyclic aromatic hydrocarbons in sediments from Michigan inland lakes[J].Environmental Science&Technology,2005,39(13):4700-4706.
[21] 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,2007,41(1):168-176.
[22] GUO Zhigang,LIN Tian,ZHANG Gan,et al. High-resolution depositional records of polycyclic aromatic hydrocarbons in the central continental shelf mud of the East China Sea[J].Environmental Science&Technology,2006,40(17):5304-5311.
[23] PAATERO P,TAPPER U. Positive matrix factorization:a nonnegative factor model with optimal utilization of error estimates of data values[J].Environmetrics,1994,5:111-126.
[24] KATSOYIANNIS A,TERZI E,CAI Q Y. On the use of PAH molecular diagnostic ratios in sewage sludge for the understanding of the PAH sources. is this use appropriate?[J]. Chemosphere,2007,69(8):1337-1339.
[25] PING L F,LUO Y M,ZHANG H B,et al.Distribution of polycyclic aromatic hydrocarbons in thirty typical soil profiles in the Yangtze River Delta Region,East China[J].Environmental Pollution,2007,147(2):358-365.
[26] ZUO Q,DUAN Y H,YANG Y,et al. Source apportionment of polycyclic aromatic hydrocarbons in surface soil in Tianjin,China[J].Environmental Pollution,2007,147(2):303-310.
[27]胡雄星,周亚康,韩中豪,等.黄浦江表层沉积物中多环芳烃的分布特征及来源[J].环境化学,2005,24(6):703-706.HU Xiongxing,ZHOU Yakang,HAN Zhonghao,et al. Distribution and source of polycyclic aromatic hydrocarbons(PAHs)in surface sediment of Huangpu River[J].Environmental Chemistry,2005,24(6):703-706.
[28] 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.
[29]张宜升,张厚勇,栾胜基,等.生物质露天焚烧及家庭燃用的多环芳烃排放特征研究[J].中国环境科学,2015,35(2):387-395.ZHANG Yisheng,ZHANG Houyong,LUAN Shengji,et al.Emission characteristics of PAHs from open and residential biomass burning[J].China Environmental Science,2015,35(2):387-395.
[30] DENG W,LI X G,LI S Y,et al.Source apportionment of polycyclic aromatic hydrocarbons in surface sediment of mud areas in the East China Sea using diagnostic ratios and factor analysis[J]. Marine Pollution Bulletin,2013,70(1/2):266-273.
[31] LARSEN R K,BAKER J E. Source apportionment of polycyclic aromatic hydrocarbons in the urban atmosphere:a comparison of three methods[J]. Environmental Science&Technology,2003,37(9):1873-1881.
[32] WANG D G,YANG M,JIA H L,et al. Polycyclic aromatic hydrocarbons in urban street dust and surface soil:comparisons of concentration,profile,and source[J]. Archives of Environmental Contamination and Toxicology,2009,56(2):173-180.
[33] LI A,JANG J K,SCHEFF P A. Application of EPA CMB 8. 2model for source apportionment of sediment PAHs in Lake Calumet,Chicago[J]. Environmental Science&Technology,2003,37(13):2958-2965.
[2] BARAKAT A O,MOSTAFA A,WADE T L,et al. Spatial distribution and temporal trends of polycyclic aromatic hydrocarbons(PAHs)in sediments from Lake Maryut,Alexandria,Egypt[J].Water,Air and Soil Pollution,2011,218:63-80.
[3]李宽,周家斌,袁畅,等.武汉市大气PM2. 5中多环芳烃的分布特征及来源[J].环境科学研究,2018,31(4):648-656.LI Kuan,ZHOU Jiabin,YUAN Chang,et al. Characteristics and source apportionment of polycyclic aromatic hydrocarbons in atmospheric PM2. 5of Wuhan City,China[J]. Research of Environmental Sciences,2018,31(4):648-656.
[4]孙小静,石纯,许世远,等.上海北部郊区土壤多环芳烃含量及来源分析[J].环境科学研究,2008,21(4):140-144.SUN Xiaojing,SHI Chun,XU Shiyuan,et al. Concentration and sources of polycyclic aromatic hydrocarbons in surface soil of north suburban Shanghai,China[J]. Research of Environmental Sciences,2008,21(4):140-144.
[5] MENZIE C A,POTOKI B B,SANTODOMATO J. Exposure to carcinogenic PAHs in the environment[J]. Environmental Science&Technology,1992,26(7):1278-1284.
[6]宁怡,柯用春,邓建才,等.巢湖表层沉积物中多环芳烃分布特征及来源[J].湖泊科学,2012,24(6):891-898.NING Yi,KE Yongchun,DENG Jiancai,et al. Distribution and sources of polycyclic aromatic hydrocarbons(PAHs)in surface sediment in Lake Chaohu[J].Lake Sciences,2012,24(6):891-898.
[7]朱春贤.滇池及其流域的经营管理问题[J].环境科学导刊,2010,29(5):25-28.ZHU Chunxian. Management and administration of Dianchi Basin[J].Environmental Science Survey,2010,29(5):25-28.
[8]李珊英,陶玉强,姚书春,等.我国湖泊沉积物多环芳烃的分布特征及来源分析[J].第四纪研究,2015,35(1):118-130.LI Shanying,TAO Yuqiang,YAO Shuchun,et al. Distribution and sources of polycyclic aromatic hydrocarbons(PAHs)in lake sediments from China[J].Quaternary Sciences,2015,35(1):118-130.
[9]任真臻,付伟.松华坝水库水质变化趋势与防护措施研究[J].环境科学导刊,2017,36(1):18-20.REN Zhenzhen,FU Wei.Trend analysis of water quality and water pollution control of Songhuaba Reservoir[J].Environmental Science Survey,2017,36(1):18-20.
[10]许正雄,夏云红.松华坝水源保护区自然地理要素综合分析[J].云南师范大学学报,1992,12(3):123-128.XU Zhengxiong,XIA Yunhong. Synthesis analysis on natural georaphy's key elements of Song-Hua-Dam source of water proecoion region[J]. Journal of Yunnan Normal University,1992,12(3):123-128.
[11]邬莉,陈静,朱晓东,等.农村秸秆焚烧的原因及对策研究[J].中国人口·资源与环境,2001,11(51):110-112.WU Li,CHEN Jing,ZHU Xiaodong,et al. Straw-burning in rural areas of China:causes and controlling strategy[J]. China Population,Resources and Environment,2001,11(51):110-112.
[12]赵语.松华坝水源区保护研究[D].昆明:云南大学,2015:1-49.
[13]赵中昆.松华坝库区水污染与防治研究[J].云南环境科学,2005,24(3):46-47.ZHAO Zhongkun. Research on controlling water pollution of Songhuaba Reservoir[J].Yunnan Environmental Science,2005,24(3):46-47.
[14]沈成达.松华坝水源保护区应实行以林为主林、农、牧、副结合的产业结构[R].昆明:林业局国家林业局昆明勘察设计院,1990:37-38.
[15]郭建阳,廖海清,韩梅,等.密云水库沉积物中多环芳烃的垂直分布、来源及生态风险评估[J].环境科学,2010,31(3):626-631.GUO Jianyang,LIAO Haiqing,HAN Mei,et al. Temporal distribution,sources,and risk assessment of polycyclic aromatic hydrocarbons in sediment core from Miyun Reservoir[J].Environmental Science,2010,31(3):626-631.
[16]赵健,周怀东,富国,等.河北西大洋水库沉积物中多环芳烃的分布、来源及生态风险评价[J].湖泊科学,2011,23(5):701-707.ZHAO Jian,ZHOU Huaidong,FU Guo,et al. Distributions,sources and ecological risk assessment of polycyclic aromatic hydrocarbons in sediments from Xidayang Reservoir,Hebei Province[J]. Lake Sciences,2011,23(5):701-707.
[17]孙盼盼,谢标,周迪,等.滇池流域宝象河水库沉积物中多环芳烃的垂直分布特征及来源解析[J].环境科学学报,2016,36(10):3615-3622.SUN Panpan,XIE Biao,ZHOU Di,et al. Vertical profile and sources of polycyclic aromatic hydrocarbons in a sediment core from Baoxianghe Reservoir in Dianchi Watershed[J]. Acta Scientiae Circumstantiae,2016,36(10):3615-3622.
[18]李秋华,郭建阳,朱元荣,等.滇池PAHs的沉积记录、来源及其生态风险评估[J].环境科学学报,2013,33(9):2565-2572.LI Qiuhua,GUO Jianyang,ZHU Yuanrong,et al. Sedimentary record,sources and risk assessment of polycyclic aromatic hydrocarbons in Dianchi Lake,southwest China[J]. Acta Scientiae Circumstantiae,2013,33(9):2565-2572.
[19] FERNANDES M B,SICRE M A,BOIREAU A. et al. Polyaromatic hydrocarbon(PAH)distributions in the Seine River and its estuary[J].Marine Pollution Bulletin,1997,34(11):857-867.
[20] KANNAN K,JOHNSON-RESTREPO B,YOHN S S,et al. Spatial and temporal distribution of polycyclic aromatic hydrocarbons in sediments from Michigan inland lakes[J].Environmental Science&Technology,2005,39(13):4700-4706.
[21] 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,2007,41(1):168-176.
[22] GUO Zhigang,LIN Tian,ZHANG Gan,et al. High-resolution depositional records of polycyclic aromatic hydrocarbons in the central continental shelf mud of the East China Sea[J].Environmental Science&Technology,2006,40(17):5304-5311.
[23] PAATERO P,TAPPER U. Positive matrix factorization:a nonnegative factor model with optimal utilization of error estimates of data values[J].Environmetrics,1994,5:111-126.
[24] KATSOYIANNIS A,TERZI E,CAI Q Y. On the use of PAH molecular diagnostic ratios in sewage sludge for the understanding of the PAH sources. is this use appropriate?[J]. Chemosphere,2007,69(8):1337-1339.
[25] PING L F,LUO Y M,ZHANG H B,et al.Distribution of polycyclic aromatic hydrocarbons in thirty typical soil profiles in the Yangtze River Delta Region,East China[J].Environmental Pollution,2007,147(2):358-365.
[26] ZUO Q,DUAN Y H,YANG Y,et al. Source apportionment of polycyclic aromatic hydrocarbons in surface soil in Tianjin,China[J].Environmental Pollution,2007,147(2):303-310.
[27]胡雄星,周亚康,韩中豪,等.黄浦江表层沉积物中多环芳烃的分布特征及来源[J].环境化学,2005,24(6):703-706.HU Xiongxing,ZHOU Yakang,HAN Zhonghao,et al. Distribution and source of polycyclic aromatic hydrocarbons(PAHs)in surface sediment of Huangpu River[J].Environmental Chemistry,2005,24(6):703-706.
[28] 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.
[29]张宜升,张厚勇,栾胜基,等.生物质露天焚烧及家庭燃用的多环芳烃排放特征研究[J].中国环境科学,2015,35(2):387-395.ZHANG Yisheng,ZHANG Houyong,LUAN Shengji,et al.Emission characteristics of PAHs from open and residential biomass burning[J].China Environmental Science,2015,35(2):387-395.
[30] DENG W,LI X G,LI S Y,et al.Source apportionment of polycyclic aromatic hydrocarbons in surface sediment of mud areas in the East China Sea using diagnostic ratios and factor analysis[J]. Marine Pollution Bulletin,2013,70(1/2):266-273.
[31] LARSEN R K,BAKER J E. Source apportionment of polycyclic aromatic hydrocarbons in the urban atmosphere:a comparison of three methods[J]. Environmental Science&Technology,2003,37(9):1873-1881.
[32] WANG D G,YANG M,JIA H L,et al. Polycyclic aromatic hydrocarbons in urban street dust and surface soil:comparisons of concentration,profile,and source[J]. Archives of Environmental Contamination and Toxicology,2009,56(2):173-180.
[33] LI A,JANG J K,SCHEFF P A. Application of EPA CMB 8. 2model for source apportionment of sediment PAHs in Lake Calumet,Chicago[J]. Environmental Science&Technology,2003,37(13):2958-2965.