三峡水库支流汝溪河河口水体汞的时空变化特征
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摘要
为探究三峡水库水位调度过程中支流河口汞的变化特征,选取三峡库区腹心地带的典型支流汝溪河河口为研究区域,设置4个断面,分别于蓄水期(9～10月)、淹没期(11～12月)、退水期(2～3月)及落干期(5～6月)这4个时期分层采集水样,分析了水样中的总汞(THg)、颗粒态汞(PHg)、溶解态汞(DHg)、活性汞(RHg)、总甲基汞(TMeHg)及溶解态甲基汞(DMeHg).结果表明,汝溪河口区域THg和TMeHg的质量浓度与中国其它水库或天然水体相接近.不同深度水体中DHg和TMeHg的质量浓度存在显著性差别,其原因是水体中的DHg和TMeHg可能来源于沉积物的再悬浮.对比同时期不同断面各形态汞质量浓度的差别,发现蓄水期长江干流来水方向的不同将导致河口区域THg和PHg的质量浓度分布不均;退水期河口水体中的颗粒物会吸附并携带大量的PHg,导致水体中THg的质量浓度明显高于其它时期.水位较为稳定的淹没期和落干期TMeHg的质量浓度明显高于其它两个时期,表明稳定的水位可能更有利于水体中甲基汞的积累,而水体的剧烈扰动会明显降低水体中TMeHg的质量浓度.
Four typical estuaries located in the Ruxi River,a tributary of the Yangtze River,were selected to investigate the possibility of mercury pollution in tributary estuaries from the Three Gorges reservoir water storage. Water samples were collected during the water storage period( September to October),the flooding period( November to December),the water withdrawal period( February to March),and the drying period( May to June) to determine the levels of mercury species including total mercury( THg),particulate mercury( PHg),dissolved mercury( DHg),reactive mercury( RHg),total methylmercury( TMeHg) and dissolved methylmercury( DMeHg). The results showed that the concentration of THg and TMeHg in the estuary of the Ruxi River was comparable with that of other reservoirs or natural waters in China. There was a significant difference in the concentration of DHg and TMeHg in the water at different depths,because DHg and TMeHg might be derived from the release of sediment to the overlying water. Comparing the concentrations of different mercury species in the four estuaries during the same period,it was found that the difference of water flow direction during the water storage period could lead to an uneven concentration distribution of THg and PHg in the estuary areas. During the water withdrawal period,the particles in the estuary water could adsorb and carry a large amount of PHg,resulting in higher THg concentration in the water in comparison with other periods. The concentration of TMeHg in the flooding and the drying periods was higher than in the other two periods,indicating that the stable water level might be conducive to the accumulation of methylmercury in the water,and the severe disturbance of the water level could significantly reduce the concentration of TMeHg in the water.
Four typical estuaries located in the Ruxi River,a tributary of the Yangtze River,were selected to investigate the possibility of mercury pollution in tributary estuaries from the Three Gorges reservoir water storage. Water samples were collected during the water storage period( September to October),the flooding period( November to December),the water withdrawal period( February to March),and the drying period( May to June) to determine the levels of mercury species including total mercury( THg),particulate mercury( PHg),dissolved mercury( DHg),reactive mercury( RHg),total methylmercury( TMeHg) and dissolved methylmercury( DMeHg). The results showed that the concentration of THg and TMeHg in the estuary of the Ruxi River was comparable with that of other reservoirs or natural waters in China. There was a significant difference in the concentration of DHg and TMeHg in the water at different depths,because DHg and TMeHg might be derived from the release of sediment to the overlying water. Comparing the concentrations of different mercury species in the four estuaries during the same period,it was found that the difference of water flow direction during the water storage period could lead to an uneven concentration distribution of THg and PHg in the estuary areas. During the water withdrawal period,the particles in the estuary water could adsorb and carry a large amount of PHg,resulting in higher THg concentration in the water in comparison with other periods. The concentration of TMeHg in the flooding and the drying periods was higher than in the other two periods,indicating that the stable water level might be conducive to the accumulation of methylmercury in the water,and the severe disturbance of the water level could significantly reduce the concentration of TMeHg in the water.
引文
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[29]赵健,毕春娟,陈振楼,等.动力和盐度影响下长江口近岸沉积物中汞的再悬浮行为[J].中国科学:化学,2011,41(1):105-116.Zhao J,Bi C J,Chen Z L,et al.Effect of dynamic and salinity conditions on activities of Hg during sediment resuspension event in the Yangtze Estuary[J].Scientia Sinica Chimica,2011,41(1):105-116.
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[31]程柳,麻冰涓,周伟立,等.三门峡水库水体中不同形态汞的分布特征[J].环境科学,2017,38(12):5032-5038.Cheng L,Ma B J,Zhou W L,et al.Distribution of different mercury species in the waterbody at Sanmenxia Reservoir[J].Environmental Science,2017,38(12):5032-5038.
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[2]Guimaraes J R D,Meili M,Malm O,et al.Hg methylation in sediments and floating meadows of a tropical lake in the Pantanal floodplain,Brazil[J].Science of the Total Environment,1998,213(1-3):165-175.
[3]黄秀山.三峡库区水污染及其治理对策[J].重庆大学学报(自然科学版),2002,25(6):155-158.Huang X S.Water pollution and counter-measures in the Three Gorges Dam Area[J].Journal of Chongqing University(Natural Science Edition),2002,25(6):155-158.
[4]张晟.三峡库区水体中营养盐与浮游生物量分布特征[D].重庆:西南农业大学,2005.Zhang S.Distribution of nutrient and plankton mass in Three Gorges Reservoir water body[D].Chongqing:Southwest Agricultural University,2005.
[5]Montgomery S,Lucotte M,Pichet P,et al.Total dissolved mercury in the water column of several natural and artificial aquatic systems of Northern Quebec(Canada)[J].Canadian Journal of Fisheries and Aquatic Sciences,1995,52(11):2483-2492.
[6]Pestana I A,Bastos W R,Almeida M G,et al.Spatial-temporal dynamics and sources of total Hg in a hydroelectric reservoir in the Western Amazon,Brazil[J].Environmental Science and Pollution Research,2016,23(10):9640-9648.
[7]Noh S,Kim C K,Kim Y,et al.Assessing correlations between monomethylmercury accumulation in fish and trophic states of artificial temperate reservoirs[J].Science of the Total Environment,2017,580:912-919.
[8]Cossa D,Gobeil C.Mercury speciation in the lower St.Lawrence Estuary[J].Canadian Journal of Fisheries and Aquatic Sciences,2000,57(S1):138-147.
[9]Bowles K C,Apte S C,Maher W A,et al.Mercury cycling in lake Gordon and lake Pedder,Tasmania(Australia).I:In-lake processes[J].Water,Air,and Soil Pollution,2003,147(1-4):3-23.
[10]Bodaly R A,St Louis V L,Paterson M J,et al.Bioaccumulation of mercury in the aquatic food chain in newly flooded areas[J].Metal Ions in Biological Systems,1997,34:259-278.
[11]Wei X,Han L F,Gao B,et al.Distribution,bioavailability,and potential risk assessment of the metals in tributary sediments of Three Gorges Reservoir:the impact of water impoundment[J].Ecological Indicators,2016,61:667-675.
[12]Bilodeau F,Therrien J,Schetagne R.Intensity and duration of effects of impoundment on mercury levels in fishes of hydroelectric reservoirs in northern Québec(Canada)[J].Inland Waters,2017,7(4):493-503.
[13]邓龙.浮游植物对汞和甲基汞的富集特征研究[D].贵阳:贵州师范大学,2016.Deng L.Enrichment features of mercury and methylmercury in Phytoplankton[D].Guiyang:Guizhou Normal University,2016.
[14]Moye H A,Miles C J,Phlips E J,et al.Kinetics and uptake mechanisms for monomethylmercury between freshwater algae and water[J].Environmental Science&Technology,2002,36(16):3550-3555.
[15]Luengen A C,Flegal A R.Role of phytoplankton in mercury cycling in the San Francisco Bay estuary[J].Limnology and Oceanography,2009,54(1):23-40.
[16]龙胜兴,何天容,陈椽,等.高原水库富营养水体浮游动物对汞的富集特征[J].中国环境科学,2017,37(1):263-270.Long S X,He T R,Chen C,et al.Characteristic of Hg accumulation by zooplankton in plateau eutrophic reservoir[J].China Environmental Science,2017,37(1):263-270.
[17]李锦秀,禹雪中,幸治国.三峡库区支流富营养化模型开发研究[J].水科学进展,2005,16(6):777-783.Li J X,Yu X Z,Xin Z G.Eutrophication model for the branch of Three-Gorges Reservoir[J].Advances in Water Science,2005,16(6):777-783.
[18]Bravo A G,Bouchet S,Tolu J,et al.Molecular composition of organic matter controls methylmercury formation in boreal lakes[J].Nature Communications,2017,8:14255.
[19]Cossa D,Sanjuan J,Noel J.Mercury transport in waters of the Strait of Dover[J].Marine Pollution Bulletin,1994,28(6):385-388.
[20]Akagi H,Malm O,Kinjo Y,et al.Methylmercury pollution in the Amazon,Brazil[J].Science of the Total Environment,1995,175(2):85-95.
[21]高建华,李军,王珍岩,等.鸭绿江河口及近岸地区沉积物中重金属分布的影响因素分析[J].地球化学,2008,37(5):430-438.Gao J H,Li J,Wang Z Y,et al.Heavy metal distribution and their influence factors in sediments of Yalu River Estuary and its adjacent sea area[J].Geochimica,2008,37(5):430-438.
[22]李仁芳,张信伟.忠县汝溪河流域水质现状调查[J].三峡环境与生态,2011,33(2):10-12.Li R F,Zhang X W.Investigation on water quality of the Ruxi River in Zhong County of Chonqing Municipality[J].Environment and Ecology in the Three Gorges,2011,33(2):10-12.
[23]李楚娴,张金洋,王定勇,等.三峡库区典型消落区土壤氮磷的动态变化特征[J].环境化学,2014,33(12):2169-2175.Li C X,Zhang J Y,Wang D Y,et al.Dynamic variations of nitrogen and phosphorous of the soil in hydro-fluctuation of Three Gorges Reservoir[J].Environmental Chemistry,2014,33(12):2169-2175.
[24]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.
[25]蒋红梅,冯新斌,梁琏,等.蒸馏-乙基化GC-CVAFS法测定天然水体中的甲基汞[J].中国环境科学,2004,24(5):568-571.Jiang H M,Feng X B,Liang L,et al.Determination of methyl mercury in waters by distillation-GC-CVAFS technique[J].China Environmental Science,2004,24(5):568-571.
[26]Bloom N.Determination of picogram levels of methylmercury by aqueous phase ethylation,followed by cryogenic gas chromatography with cold vapour atomic fluorescence detection[J].Canadian Journal of Fisheries and Aquatic Sciences,1989,46(7):1131-1140.
[27]Mason R P,Sullivan K A.Mercury and methylmercury transport through an urban watershed[J].Water Research,1998,32(2):321-330.
[28]毕春娟,陈振楼,许世远,等.河口近岸水体中颗粒态重金属的潮周期变化[J].环境科学,2006,27(1):132-136.Bi C J,Chen Z L,Xu S Y,et al.Variation of particulate heavy metals in coastal water over the course of tidal cycle in estuary[J].Environmental Science,2006,27(1):132-136.
[29]赵健,毕春娟,陈振楼,等.动力和盐度影响下长江口近岸沉积物中汞的再悬浮行为[J].中国科学:化学,2011,41(1):105-116.Zhao J,Bi C J,Chen Z L,et al.Effect of dynamic and salinity conditions on activities of Hg during sediment resuspension event in the Yangtze Estuary[J].Scientia Sinica Chimica,2011,41(1):105-116.
[30]李萍.三峡库区典型消落带水体中汞的时空分布[D].重庆:西南大学,2013.Li P.Distribution characteristics of mercury in water level fluctuating zone of Three Gorges Reservoir[D].Chongqing:Southwest University,2013.
[31]程柳,麻冰涓,周伟立,等.三门峡水库水体中不同形态汞的分布特征[J].环境科学,2017,38(12):5032-5038.Cheng L,Ma B J,Zhou W L,et al.Distribution of different mercury species in the waterbody at Sanmenxia Reservoir[J].Environmental Science,2017,38(12):5032-5038.
[32]孟博,冯新斌,陈春宵,等.乌江流域不同营养水平水库水体中汞的含量和形态分布[J].生态学杂志,2011,30(5):951-960Meng B,Feng X B,Chen C X,et al.Distribution of total mercury and methylmercury in two hydroelectric reservoirs of Guizhou Province,China[J].Chinese Journal of Ecology,2011,30(5):951-960.
[33]郑伟,康世昌,冯新斌,等.西藏雅鲁藏布江表层水中汞的形态与空间分布特征[J].科学通报,2010,55(20):2026-2032.Zheng W,Kang S C,Feng X B,et al.Mercury speciation and spatial distribution in surface waters of the Yarlung Zangbo River,Tibet[J].Chinese Science Bulletin,2010,55(24):2697-2703.
[34]Furutani A,Rudd J W M.Measurement of mercury methylation in lake water and sediment samples[J].Applied and Environmental Microbiology,1980,40(4):770-776.
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