题名基于砷、汞形态的生态风险评价研究
作者杜萌
学位类别博士
答辩日期2014-05
授予单位中国科学院研究生院
授予地点北京
导师杜宇国,魏东斌
关键词 形态 毒性 生态风险评价 arsenic mercury species toxicity ecological risk assessment
其他题名Ecological risk assessment of arsenic and mercury based on different species
学位专业环境科学
中文摘要      砷、汞是两种典型的重金属污染物,它们在自然界中以多种形态存在。由于重金属的形态不同,其毒性特征也存在较大差异,所引起的生态风险迥异。本文选取重金属污染物砷、汞为研究对象,首先收集、整理了不同形态砷、汞的毒性数据,借助物种敏感度分布等方法,计算出了不同形态砷、汞的预测无效应浓度阈值(PNECs);其次,建立了环境样品中不同形态砷、汞的液相色谱-氢化物发生-原子荧光(LC-HG-AFS)联用的检测方法;在此基础上,采集了南方某流域的环境样品,对不同形态砷、汞的污染现状进行了检测,并结合不同形态砷、汞的 PNEC值,研究了该流域环境介质中不同形态砷、汞的风险分布情况;最后,对流域内典型行业废水中砷、汞的污染情况及风险分布进行了研究,主要研究成果如下:
    (1)收集、整理了不同形态砷、汞的毒性数据,利用物种敏感度分布法(SSD)和评价因子法(AF)分别计算了三价砷(As(III))、五价砷(As(V))和一甲基砷(DMA)的 PNEC值为  43.65 μg/L、250.18  μg/L和  2.00×103 μg/L,表明了不同形态砷化合物的毒性大小依次为     As(III)>As(V)>DMA,无机汞和甲基汞的PNEC值为  0.39 μg/L和  6.5×10-3 μg/L,甲基汞的毒性大于无机汞。
      (2)通过优化前处理方法,采用  LC-HG-AFS  联用技术分别建立了不同形态砷、汞的检测方法,其中砷的四种形态在 11  min  内可实现分离检测,汞的三种形态在 7 min内实现分离检测,并均具有良好的回收率。
      (3)采集了我国南方某流域的水和沉积物样品,利用  LC-HG-AFS  联用方法检测了砷、汞的污染水平,结果显示除一、两个采样点外,不同形态砷、汞在该流域水体中的浓度均未超过地表水环境质量标准(GB  3838-2002  Ⅲ类)的浓度限值。砷在丰水期和枯水期的浓度平均值分别为 6.51 μg/L和  20.16 μg/L,其中As(III)的平均值为 10.78 μg/L和  7.89  μg/L,As(V)的平均值为 0.91 μg/L和   14.83μg/L;无机汞在丰水期和枯水期的浓度范围为  0.02  μg/L-0.14  μg/L 和  ND-0.03μg/L,平均值分别为 0.05 μg/L和  0.01 μg/L。沉积物样品中总砷的含量低于国家海洋沉积物质量标准(GB 15618-1995  I类)的浓度限值  20 mg/kg,在丰水期和枯水期 As(III)的平均值为 0.48 mg/kg和  0.29 mg/kg,As(V)的平均值为 0.47 mg/kg和 0.42 mg/kg;样品中汞的检出浓度接近或高于国家海洋沉积物质量标准的浓度限值 0.20 mg/kg,在丰水期和枯水期的浓度范围分别为 ND-2.10 mg/kg和  ND-6.14mg/kg,其中无机汞在丰水期和枯水期的平均浓度为 0.33 mg/kg和  0.39  mg/kg,甲基汞的平均浓度小于 0.01 mg/kg。
      (4)砷在该流域内的水体和沉积物介质中均为低生态风险, RQ  的平均值分别为  0.24 和 0.23;汞在该流域水体中为低风险,均为无机汞,RQ  值最大为0.36,但在沉积物中风险较高,Hg(II)和 MeHg的  RQ平均值为  14.61和  4.92,特别是在干流的下游和部分支流断面风险更高。
      (5)采集了流域内典型行业排放的废水,检测了砷、汞的排放水平。结果发现流域废水中砷的排放浓度较低。而制药、造纸、城市污水处理及电子电镀等行业废水中,汞有一定程度的排放,可能是造成汞污染的主要来源。
      综上,本研究主要针对不同形态砷、汞的毒性差异,提出了基于不同形态砷、汞的风险评价理念,克服了传统的基于总砷、总汞基础上进行生态风险评价的不足,可以更加准确的评价环境中砷、汞污染所造成的潜在生态风险。本研究将为有关部门制定相应的环境保护规划提供科学依据。
英文摘要      Arsenic (As)  and mercury (Hg)  are two kinds  of typical  heavy metal pollutants.They  exist  in  different chemical  species  in  the  environment.  Due  to  the different chemical species of heavy mental, the toxicity and ecological risk they caused are also different.  So  arsenic and  mercury  were  selected  as  research  objects in  this  study.Firstly, the toxicity data of arsenic and mercury  on different species were selected, the predicted no-effect concentrations  (PNECs) of them were  calculated according to the species  sensitivity   distribution   (SSD)  method.   Then  the   liquid  chromatography hydride-generation    atomic   fluorescence    spectrometry   (LC-HG-AFS)    detection method  was established.  On  this  basis, the  environmental  samples  of certain  river basin in  southern China  were  collected. And  the pollution  characteristics of  arsenic and mercury on different species  were analysed, then basing on the PNECs  of arsenic and mercury,  the risk  distribution of  them in certain  river basin  was studied.  Lastly, the pollution distribution characteristics and ecological risk  of arsenic and mercury on different species in the wastewater of representative industry were explored. The main works carried out in this research are as follows:
      (1) The  toxicity data of  arsenic and mercury  on different species  were selected, then the PNEC values of As(III), As(V), and DMA were 43.65 μg/L, 250.18 μg/L, and 2.00×103 μg/L according  to the species sensitivity  distribution (SSD) and assessment factor  (AF)  methods. The  result  indicated  that  the  toxicity  of different  species  of arsenic was As(III)>As(V)>DMA;  the PNEC values of  Hg(II) and methyl mercury (MeHg)  were 0.39  μg/L  and  6.5×10-3 μg/L,  the  result  showed  that the  toxicity  of MeHg was much higher than Hg(II).
      (2)   By    optimizing   the   pre-treatment    method,   the    detection   method    of LC-HG-AFS about  different species  of  arsenic and  mercury was  established. Using this method, the four forms  of arsenic could be separated within 11 minutes,  the three forms  of mercury  could  be separated  within  7 minutes.  The  average recovery  was good.
      (3) The water and sediment samples in certain river basin in southern China were collected,  and  the  pollution distribution  of  arsenic  and  mercury  were  detected  by LC-HG-AFS method. The  results showed that  except for individual  sampling points, the concentration  of arsenic  and mercury  in water of  this river  basin was  below the limit   value  of   the   Chinese  environmental   quality   standards  for   surface   water (GB3838-2002, ClassⅢ).   The  average concentrations  of arsenic  in wet  season and dry   season   were   6.51   μg/L   and  20.16   μg/L,   respectively.   And   the   average concentration of  As(III) was 10.78 μg/L  and 7.89 μg/L,  the average concentration  of As(V) was  0.91 μg/L and 14.83  μg/L. The concentration  range of inorganic  mercury in  wet   season  and   dry   season  were   0.02  μg/L-0.14   μg/L  and   ND-0.03  μg/L,respectively.  And  the  average  concentrations were  0.05  μg/L  and  0.01  μg/L.  The concentrations of total  arsenic in sediments were below the  limit value (20 mg/kg) of the  Chinese  environmental  quality standard  for  soils (GB15618-1995  Class  I). The average concentrations of  As(III) in wet season  and dry season were  0.48 mg/kg and 0.29  mg/kg,  and  the  average concentrations  of  As(V)  were  0.47  mg/kg  and  0.42 mg/kg. The  concentrations  of mercury  in sediments  were close  to or  a  little higher than the  limit value  (0.20 mg/kg) of  the Chinese  environmental quality  standard for soils.  The  concentration  ranges   of  mercury  in  wet  season  and   dry  season  were ND-2.10 mg/kg and  ND-6.14 mg/kg, respectively. And the  average concentrations of inorganic mercury in wet season and dry season were  0.33 mg/kg and 0.39 mg/kg, the average concentration of MeHg was lower than 0.01 mg/kg.
      (4) There was a low risk  from arsenic in water and sediments in the studied  river basin,  and the  average  values of  RQ  were 0.24  and  0.23  respectively. The  risk  of inorganic mercury  in water was  low, the maximum  value of RQ was  0.36. But there was a high risk  of mercury in sediments, the  average RQ values of  Hg(II) and MeHg were 14.61 and 4.92 respectively. And  the ecological risk was much higher especially on the downstream side of the river basin and part of the tributaries.
      (5) The  wastewater discharged  by representative  industry in  certain river  basin was collected  and the  pollution distributions  of arsenic  and mercury  were analysed. The  results  showed   that  the  concentrations   of  arsenic  in   wastewater  were  low. Pharmacy, paper  making, urban  sewage treatment  and electronic  industry should  be the main source of mercury pollution.
      In  conclusion, because  that  the  toxicities  of arsenic  and  mercury on  different species are not  the same, the idea  that ecological risk  assessment should be based  on
arsenic and mercury  with different species was  proposed. Comparing with traditional ecological   risk  assessment   method   focused  on   total   arsenic  and   mercury,   the
ecological risk assessment of arsenic  and mercury based on different species could be much more accurate. The  study provides a scientific basis for relevant  departments to formulate the corresponding environmental protection planning.
公开日期2015-07-07
内容类型学位论文
源URL[http://ir.rcees.ac.cn/handle/311016/15642]  
专题生态环境研究中心_环境化学与生态毒理学国家重点实验室
推荐引用方式
GB/T 7714
杜萌. 基于砷、汞形态的生态风险评价研究[D]. 北京. 中国科学院研究生院. 2014.
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