唐山陡河水库沉积物汞的分布、来源及污染评价
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摘要
为弄清陡河燃煤电厂大气汞沉降对毗邻的陡河水库沉积物中总汞、甲基汞的贡献及其污染程度,于2013年8月对陡河水库沉积物进行了采样,测定了沉积物中总汞、甲基汞、有机质以及孔隙水中溶解态汞含量等参数,运用地累积指数法评价了陡河水库沉积物的汞污染现状和污染程度.结果表明,陡河水库沉积物中总汞含量(dw)范围为19~97 ng·g~(-1),甲基汞含量(dw)范围为0.02~1.27 ng·g~(-1),均表现为表层高于底层,说明陡河水库沉积物的汞含量正逐年升高,外源汞输入对陡河沉积物负荷产生了一定的影响.受电厂大气汞干湿沉降影响,陡河水库周边土壤汞含量(dw)平均值为22 ng·g~(-1),而陡河水库3个沉积物柱库心总汞含量最高,其次为西支,东支最低.结合上游大黑汀水库较高的沉积物汞含量(总汞平均值为176 ng·g~(-1)),以及陡河水库附近较低的土壤汞含量,初步判断陡河水库沉积物中汞的主要来源为大黑汀水库的高汞水源输入,电厂汞沉积输入贡献相对较小.陡河沉积物总汞、甲基汞与有机质之间均呈显著的正相关关系,表明沉积物中有机质具有较好的吸附总汞和甲基汞的能力,并对甲基汞产生具有重要作用.地累积指数Igeo的评价结果表明,陡河水库各点位沉积物的汞污染程度依次为库心>西支>东支,库心和西支属于中度污染,东支属于轻微污染.大黑汀水库受周边采矿企业影响,两个采样点沉积物的地累积指数污染评价属于中强污染和强污染.
Sediment cores from Douhe reservoir in Tangshan City were sampled in August 2013,in order to evaluate the mercury( Hg)pollution degree and its possible sources. Agriculture soils surrounding the Douhe reservoir and sediments from an upstream reservoir( Daheiting) were also collected. Total mercury( THg),methylmercury( Me Hg),dissolved mercury in pore water( DHg) and organic matter( OM) in sediment of Douhe reservoir were analyzed,while,only THg in the agriculture soils and upstream reservoir sediments was determined. Finally,the geoaccumulation index method was applied to evaluate the Hg pollution status in soils and reservoir sediments. The results showed that THg content in sediment of Douhe reservoir ranged from 19 to 97 ng·g~(-1). dw,Me Hg( dw) from0. 02 to 1. 27 ng·g~(-1),and the contents of both THg and Me Hg were higher in the upper layers than the deeper layers,indicating that Hg in sediments was increasing in recent years by the exogenetic loadings. THg( dw) in soils offshore the Douhe reservoir,which is close to a large coal-fired power plant,averaged at 22 ng·g~(-1). Among the three sediment cores of Douhe reservoir,the central point had the highest THg,followed by the western site,and the eastern site had the lowest THg. While,THg content( dw) in sediments of Daheiting reservoir was much higher,with a mean of 176 ng·g~(-1). Combining all the above information,we concluded that Hg in Douhe reservoir was mainly derived from the Daheiting reservoir and the mercury atmospheric deposition from the nearby coal-fired power plant contributed a less content. THg and Me Hg in the sediments of Douhe reservoir were positively correlated with OM,indicating that OM in sediments had good ability of adsorbing THg and Me Hg,and also played an important role in Hg methylation.The geoaccumulation index( Igeo) showed that the Hg pollution status deceased in this order: central of Daheting,Daba of Daheting,central of Douhe,western of Douhe,eastern of Douhe,soils surrounding Douhe. Central and western sites in Douhe belonged to moderate pollution and the eastern site belonged to slight pollution. While,sediments of Daheiting reservoir,affected by the iron oremining activities,were in the moderate and strong pollution status.
Sediment cores from Douhe reservoir in Tangshan City were sampled in August 2013,in order to evaluate the mercury( Hg)pollution degree and its possible sources. Agriculture soils surrounding the Douhe reservoir and sediments from an upstream reservoir( Daheiting) were also collected. Total mercury( THg),methylmercury( Me Hg),dissolved mercury in pore water( DHg) and organic matter( OM) in sediment of Douhe reservoir were analyzed,while,only THg in the agriculture soils and upstream reservoir sediments was determined. Finally,the geoaccumulation index method was applied to evaluate the Hg pollution status in soils and reservoir sediments. The results showed that THg content in sediment of Douhe reservoir ranged from 19 to 97 ng·g~(-1). dw,Me Hg( dw) from0. 02 to 1. 27 ng·g~(-1),and the contents of both THg and Me Hg were higher in the upper layers than the deeper layers,indicating that Hg in sediments was increasing in recent years by the exogenetic loadings. THg( dw) in soils offshore the Douhe reservoir,which is close to a large coal-fired power plant,averaged at 22 ng·g~(-1). Among the three sediment cores of Douhe reservoir,the central point had the highest THg,followed by the western site,and the eastern site had the lowest THg. While,THg content( dw) in sediments of Daheiting reservoir was much higher,with a mean of 176 ng·g~(-1). Combining all the above information,we concluded that Hg in Douhe reservoir was mainly derived from the Daheiting reservoir and the mercury atmospheric deposition from the nearby coal-fired power plant contributed a less content. THg and Me Hg in the sediments of Douhe reservoir were positively correlated with OM,indicating that OM in sediments had good ability of adsorbing THg and Me Hg,and also played an important role in Hg methylation.The geoaccumulation index( Igeo) showed that the Hg pollution status deceased in this order: central of Daheting,Daba of Daheting,central of Douhe,western of Douhe,eastern of Douhe,soils surrounding Douhe. Central and western sites in Douhe belonged to moderate pollution and the eastern site belonged to slight pollution. While,sediments of Daheiting reservoir,affected by the iron oremining activities,were in the moderate and strong pollution status.
引文
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[9]赵庆令,李清彩,谢江坤,等.应用富集系数法和地累积指数法研究济宁南部区域土壤重金属污染特征及生态风险评价[J].岩矿测试,2015,34(1):129-137.Zhao Q L,Li Q C,Xie J K,et al.Characteristics of soil heavy metal pollution and its ecological risk assessment in South Jining district using methods of enrichment factor and index of geoaccumulation[J].Rock and Mineral Analysis,2015,34(1):129-137.
[10]王红亚,石元春,于澎涛,等.河北平原南部曲周地区河间洼地沉积若干特征及相关问题——对吴忱等问题的回答[J].第四纪研究,2004,24(1):105-109.Wang H Y,Shi Y C,Yu P T,et al.Some characteristics of the interchannl-depression deposits in Quzhou Area,the Southern Hebei Plain and relevant issues:a reply to Wu Chen et al[J].Quaternary Sciences,2004,24(1):105-109.
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[12]张雅慧,张成,王定勇,等.典型钢铁行业汞排放特征及质量平衡[J].环境科学,2015,36(12):4366-4373.Zhang Y H,Zhang C,Wang D Y,et al.Characteristic of mercury emissions and mass balance of the typical iron and steel industry[J].Environmental Science,2015,36(12):4366-4373.
[13]王立卿,宋秋波.潘家口、大黑汀水库水源地保护对策研究[J].海河水利,2007,(4):21-23,27.
[14]Lohman K,Seigneur C,Edgerton E,et al.Modeling mercury in power plant plumes[J].Environmental Science&Technology,2006,40(12):3848-3854.
[15]Seigneur C,Vijayaraghavan K,Lohman K.Atmospheric mercury chemistry:sensitivity of global model simulations to chemical reactions[J].Journal of Geophysical Research:Atmospheres,2006,111(D22):D22306.
[16]Wu G H,Wei Z,Su R X.Distribution,accumulation and mobility of mercury in superficial sediment samples from Tianjin,northern China[J].Journal of Environmental Monitoring,2011,13(9):2488-2495.
[17]Sanei H,Goodarzi F,Outridge P M.Spatial distribution of mercury and other trace elements in recent lake sediments from central Alberta,Canada:an assessment of the regional impact of coal-fired power plants[J].International Journal of Coal Geology,2010,82(1-2):105-115.
[18]陈吉,李秋华,李仲根,等.河北省衡水湖沉积物中汞的分布特征及生态风险[J].生态毒理学报,2014,9(5):908-915.Chen J,Li Q H,Li Z G,et al.Distribution and risk assessment of mercury in the sediments of Hengshuihu Lake,Hebei Province[J].Asian Journal of Ecotoxicology,2014,9(5):908-915.
[19]潘鲁生,刘秀伟,石春梅,等.乌江流域东风水库沉积物中汞及甲基汞的时空分布特征[J].地球与环境,2012,40(2):201-207.Pan L S,Liu X W,Shi C M,et al.Spatial and temporal distribution of mercury and methylmercury in sediments of the Dongfeng reservoir,Guizhou Province[J].Earth and Environment,2012,40(2):201-207.
[20]Wang S F,Xing D H,Jia Y F,et al.The distribution of total mercury and methyl mercury in a shallow hypereutrophic lake(Lake Taihu)in two Seasons[J].Applied Geochemistry,2012,27(1):343-351.
[21]Feng X B,Jiang H M,Qiu G L,et al.Geochemical processes of mercury in Wujiangdu and Dongfeng Reservoirs,Guizhou,China[J].Environmental Pollution,2009,157(11):2970-2984.
[22]何天容,冯新斌,郭艳娜,等.红枫湖沉积物中汞的环境地球化学循环[J].环境科学,2008,29(7):1768-1774.He T R,Feng X B,Guo Y N,et al.Geochemical cycling of mercury in the sediment of Hongfeng Reservior[J].Environmental Science,2008,29(7):1768-1774.
[23]Yan H Y,Feng X B,Shang L H,et al.The variations of mercury in sediment profiles from a historically mercurycontaminated reservoir,Guizhou Province,China[J].Science of the Total Environment,2008,407(1):497-506.
[24]白薇扬.阿哈水库中不同形态汞迁移转化规律的初步探讨[D].贵阳:中国科学院地球化学研究所,2006.Bai W Y.The primary study on the distributions and transformations of the different species mercury in Aha Reservoir[D].Guiyang:Institute of Geochemistry,Chinese Academy of Sciences,2006.
[25]Gray J E,Hines M E.Biogeochemical mercury methylation influenced by reservoir eutrophication,Salmon Falls Creek Reservoir,Idaho,USA[J].Chemical Geology,2009,258(3-4):157-167.
[26]Hines N A,Brezonik P L,Engstrom D R.Sediment and porewater profiles and fluxes of mercury and methylmercury in a small seepage lake in Northern Minnesota[J].Environmental Science&Technology,2004,38(24):6610-6617.
[27]刘凯,杨芳,冯新斌,等.贵州省普定水库水体及沉积物孔隙水中汞的含量和形态分布初步研究[J].矿物岩石地球化学通报,2009,28(3):239-247.Liu K,Yang F,Feng X B,et al.Concentrations and species distributions of mercury in water and sediment porewater of Puding Reservoir,Guizhou Province[J].Bulletin of Mineralogy,Petrology and Geochemistry,2009,28(3):239-247.
[28]覃东立,姜海峰,黄晓丽,等.松花江沉积物汞的新变化:分布、演化与现状及潜在生态风险评估[J].环境科学学报,2016,36(6):1910-1916.Qin D L,Jiang H F,Huang X L,et al.Changes of total mercury in sediments from Songhua River:distribution,evolution and potential ecological risk[J].Acta Scientiae Circumstantiae,2016,36(6):1910-1916.
[29]李莹杰,张列宇,吴易雯,等.江苏省浅水湖泊表层沉积物重金属GIS空间分布及生态风险评价[J].环境科学,2016,37(4):1321-1329.Li Y J,Zhang L Y,Wu Y W,et al.GIS spatial distribution and ecological risk assessment of heavy metals in surface sediments of shallow lakes in Jiangsu Province[J].Environmental Science,2016,37(4):1321-1329.
[2]王雨春,黄荣贵,万国江.SWB-1型便携式湖泊沉积物—界面水取样器的研制[J].地质地球化学,1998,(1):94-96.Wang Y C,Huang R G,Wan G J.A newly developed sampler for collecting samples near the lacustrine sediment—water interface[J].Geology-Geochemistry,1998,(1):94-96.
[3]王翠萍,闫海鱼,刘鸿雁,等.使用Lumex测汞仪快速测定固体样品中总汞的方法[J].地球与环境,2010,38(3):378-382.Wang C P,Yan H Y,Liu H Y,et al.The method of rapidly measuring total mercury in solid samples using Lumex analytical equipment[J].Earth and Environment,2010,38(3):378-382.
[4]何天容,冯新斌,戴前进,等.萃取-乙基化结合GC-CVAFS法测定沉积物及土壤中的甲基汞[J].地球与环境,2004,32(2):83-86.He T R,Feng X B,Dai Q J,et al.Determination of methyl mercury in sediments and soils by GC-CVAFS after aqueous phase ethylation[J].Earth and Environment,2004,32(2):83-86.
[5]阎海鱼,冯新斌,商立海,等.天然水体中痕量汞的形态分析方法研究[J].分析测试学报,2003,22(5):10-13.Yan H Y,Feng X B,Shang L H,et al.Speciation analysis of ultra trace levels of mercury in natural waters[J].Journal of Instrumental Analysis,2003,22(5):10-13.
[6]季天委.重铬酸钾容量法中不同加热方式测定土壤有机质的比较研究[J].浙江农业学报,2005,17(5):311-313.Ji T W.Comparison on determining the organic matter contents in the soils by different heating methods in the potassium dichromate-volumetric method[J].Acta Agriculturae Zhejiangensis,2005,17(5):311-313.
[7]Li Z G,Feng X B,Li G H,et al.Distributions,sources and pollution status of 17 trace metal/metalloids in the street dust of a heavily industrialized city of central China[J].Environmental Pollution,2013,182:408-416.
[8]蒋丽婷.河北省唐山市丰润区土壤中重金属分布及土壤质量评价[D].北京:中国地质大学(北京),2006.Jang L T.The heavy metal concentrations and soil quality evaluation in the Fengrun Region,Tangshan City,Hebei Province[D].Beijing:China University of Geosciences,2006.
[9]赵庆令,李清彩,谢江坤,等.应用富集系数法和地累积指数法研究济宁南部区域土壤重金属污染特征及生态风险评价[J].岩矿测试,2015,34(1):129-137.Zhao Q L,Li Q C,Xie J K,et al.Characteristics of soil heavy metal pollution and its ecological risk assessment in South Jining district using methods of enrichment factor and index of geoaccumulation[J].Rock and Mineral Analysis,2015,34(1):129-137.
[10]王红亚,石元春,于澎涛,等.河北平原南部曲周地区河间洼地沉积若干特征及相关问题——对吴忱等问题的回答[J].第四纪研究,2004,24(1):105-109.Wang H Y,Shi Y C,Yu P T,et al.Some characteristics of the interchannl-depression deposits in Quzhou Area,the Southern Hebei Plain and relevant issues:a reply to Wu Chen et al[J].Quaternary Sciences,2004,24(1):105-109.
[11]马权,韩光泽,赵栋华.大黑汀水库生态环境现状及保护对策[J].海河水利,2012,(6):22-23.
[12]张雅慧,张成,王定勇,等.典型钢铁行业汞排放特征及质量平衡[J].环境科学,2015,36(12):4366-4373.Zhang Y H,Zhang C,Wang D Y,et al.Characteristic of mercury emissions and mass balance of the typical iron and steel industry[J].Environmental Science,2015,36(12):4366-4373.
[13]王立卿,宋秋波.潘家口、大黑汀水库水源地保护对策研究[J].海河水利,2007,(4):21-23,27.
[14]Lohman K,Seigneur C,Edgerton E,et al.Modeling mercury in power plant plumes[J].Environmental Science&Technology,2006,40(12):3848-3854.
[15]Seigneur C,Vijayaraghavan K,Lohman K.Atmospheric mercury chemistry:sensitivity of global model simulations to chemical reactions[J].Journal of Geophysical Research:Atmospheres,2006,111(D22):D22306.
[16]Wu G H,Wei Z,Su R X.Distribution,accumulation and mobility of mercury in superficial sediment samples from Tianjin,northern China[J].Journal of Environmental Monitoring,2011,13(9):2488-2495.
[17]Sanei H,Goodarzi F,Outridge P M.Spatial distribution of mercury and other trace elements in recent lake sediments from central Alberta,Canada:an assessment of the regional impact of coal-fired power plants[J].International Journal of Coal Geology,2010,82(1-2):105-115.
[18]陈吉,李秋华,李仲根,等.河北省衡水湖沉积物中汞的分布特征及生态风险[J].生态毒理学报,2014,9(5):908-915.Chen J,Li Q H,Li Z G,et al.Distribution and risk assessment of mercury in the sediments of Hengshuihu Lake,Hebei Province[J].Asian Journal of Ecotoxicology,2014,9(5):908-915.
[19]潘鲁生,刘秀伟,石春梅,等.乌江流域东风水库沉积物中汞及甲基汞的时空分布特征[J].地球与环境,2012,40(2):201-207.Pan L S,Liu X W,Shi C M,et al.Spatial and temporal distribution of mercury and methylmercury in sediments of the Dongfeng reservoir,Guizhou Province[J].Earth and Environment,2012,40(2):201-207.
[20]Wang S F,Xing D H,Jia Y F,et al.The distribution of total mercury and methyl mercury in a shallow hypereutrophic lake(Lake Taihu)in two Seasons[J].Applied Geochemistry,2012,27(1):343-351.
[21]Feng X B,Jiang H M,Qiu G L,et al.Geochemical processes of mercury in Wujiangdu and Dongfeng Reservoirs,Guizhou,China[J].Environmental Pollution,2009,157(11):2970-2984.
[22]何天容,冯新斌,郭艳娜,等.红枫湖沉积物中汞的环境地球化学循环[J].环境科学,2008,29(7):1768-1774.He T R,Feng X B,Guo Y N,et al.Geochemical cycling of mercury in the sediment of Hongfeng Reservior[J].Environmental Science,2008,29(7):1768-1774.
[23]Yan H Y,Feng X B,Shang L H,et al.The variations of mercury in sediment profiles from a historically mercurycontaminated reservoir,Guizhou Province,China[J].Science of the Total Environment,2008,407(1):497-506.
[24]白薇扬.阿哈水库中不同形态汞迁移转化规律的初步探讨[D].贵阳:中国科学院地球化学研究所,2006.Bai W Y.The primary study on the distributions and transformations of the different species mercury in Aha Reservoir[D].Guiyang:Institute of Geochemistry,Chinese Academy of Sciences,2006.
[25]Gray J E,Hines M E.Biogeochemical mercury methylation influenced by reservoir eutrophication,Salmon Falls Creek Reservoir,Idaho,USA[J].Chemical Geology,2009,258(3-4):157-167.
[26]Hines N A,Brezonik P L,Engstrom D R.Sediment and porewater profiles and fluxes of mercury and methylmercury in a small seepage lake in Northern Minnesota[J].Environmental Science&Technology,2004,38(24):6610-6617.
[27]刘凯,杨芳,冯新斌,等.贵州省普定水库水体及沉积物孔隙水中汞的含量和形态分布初步研究[J].矿物岩石地球化学通报,2009,28(3):239-247.Liu K,Yang F,Feng X B,et al.Concentrations and species distributions of mercury in water and sediment porewater of Puding Reservoir,Guizhou Province[J].Bulletin of Mineralogy,Petrology and Geochemistry,2009,28(3):239-247.
[28]覃东立,姜海峰,黄晓丽,等.松花江沉积物汞的新变化:分布、演化与现状及潜在生态风险评估[J].环境科学学报,2016,36(6):1910-1916.Qin D L,Jiang H F,Huang X L,et al.Changes of total mercury in sediments from Songhua River:distribution,evolution and potential ecological risk[J].Acta Scientiae Circumstantiae,2016,36(6):1910-1916.
[29]李莹杰,张列宇,吴易雯,等.江苏省浅水湖泊表层沉积物重金属GIS空间分布及生态风险评价[J].环境科学,2016,37(4):1321-1329.Li Y J,Zhang L Y,Wu Y W,et al.GIS spatial distribution and ecological risk assessment of heavy metals in surface sediments of shallow lakes in Jiangsu Province[J].Environmental Science,2016,37(4):1321-1329.