柴达木盆地盐湖岩芯痕量汞的赋存形态及其环境地球化学研究
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摘要
察尔汗盐湖位于柴达木盆地中部,是中国目前最大的盐湖,也是富含多种矿物的大型综合盐湖。察尔汗盐湖岩芯沉积物记录着丰富的盐湖地质信息,通过对其样品中痕量类金属元素汞垂直分布的研究,可反演和追溯该区域内汞的迁移史,反映该地区地质变迁过程及古气候变化,同时也对该地区元素地球循环、生态效应及环境评价等研究有着重要的意义。本论文在导师主持的国家自然科学基金重点和面上项目(20836009、40773045)资助下,以察尔汗盐湖地芯样品为研究对象,首次研究了察尔汗盐湖地芯样品中汞的分布行为。
主要研究内容:①建立适用于测定盐湖地芯样品及盐湖区内高矿化度水体中汞含量的分析方法;②通过对地芯样品中的总汞(THg)、总铁(TFe)、总锰(TMn)的提取、测定及分析,揭示地芯样品中汞的垂向分布特征;③通过对地芯样品中水溶态汞(Hg-H2O)、铁锰氧化物结合态汞(Hg-oxal)、有机物结合态汞(Hg-H2O2)、硫化矿物吸附态汞(Hg-pyrite)的连续浸提与测定分析,揭示各种形态汞在岩芯样品中的垂向分布与迁移转化规律。
主要研究成果:
①通过改进氢化物发生-原子荧光法(HG-AFS)天然水体系痕量汞分析,建立了可适用于高盐度沉积物样品中汞含量的测定方法;
②察尔汗盐湖不同岩性样品中,总汞(THg)的含量大小为:黏土>淤泥>盐类物质夹粉砂>细纱质盐类>纯石盐,但研究发现,盐类物质对汞的富集作用没有特别明显的差异;
③盐湖地芯样品0 ~ -103.15 m中总汞(THg)含量的垂向分布特征为:总汞的含量由上至下呈表层(0.00 ~ -10.04 m)较高,中间区段(-10.04 ~ -40.27 m)不均一,-40.27 ~-49.65 m较低,-49.65 ~ -82.64 m增大,-82.64 ~ -103.15 m整体含量有所降低的趋势;
④察尔汗盐湖盐类矿物沉积层(0.00 m～-47.07 m)地芯样品中,THg与TFe、TMn的地球化学相关系数分别为0.41和0.36,说明在盐湖沉积层中TFe、TMn对THg的垂向含量分布具有明显影响;在湖相粉砂沉积层(-47.07 m～-103.15 m)地芯样品中,TFe、TMn对THg的地球化学相关系数分别为0.25和0.05,表明湖相沉积层铁锰氧化物对THg的垂向分布影响相对较小。总体而言,在0.00 ~-103.15 m的地芯样品中,含铁氧化物对总汞含量分布的影响大于锰氧化物对总汞分布的影响。
⑤察尔汗盐湖地芯样品中痕量汞各赋存形态的含量大小:Hg(oxal) > Hg (pyrite) > Hg(H_2O) > Hg(H_2O_2) ,说明样品中的汞主要以铁锰氧化物结合态Hg(oxal)和硫化物结合态Hg (pyrite)形式存在;水溶态汞Hg(H_2O)和有机物结合态汞Hg(H_2O_2)在地芯样品中含量极低。
Qarhan Salt Lake located in the central Qaidam Basin is the largest salt lake in China, and it has various mineral in salt lake. The vertical distribution of mercury records the earth's geological information in Qaidam Basin. It would not only demonstrate traces back on the region’s history for mercury migration, but also reflect the geological processing and fluctuation in the palaeoclimate information. The results could reveal the effect of the earth recycling, ecological and the environmental evaluation. Under the joint financial supports from the National Natural Science Foundation of China (Grants 20836009 and 40773045), the vertical distributions of mercury in Qarhan Salt Lake was carried out.
The researching contents include:①Establish a sensitive mercury analysis method for high saline brines and core samples from the salt lake;②The core example includes (expressed as THg), total iron(expressed as TFe), total manganese(expressed as TMn), were extracted determined and then were analyzed. It reveal the vertical distribution of the THg, TFe and TMn.③The Hg-H2O,Hg-oxal,Hg-H2O2 and Hg-pyrite in core samples from the salt lake, were extrated determined and then were analyzed and it reveals the various forms of mercury in the core samples in the vertical distribution and the migation regular pattern.
Solutions in this study can be summerized as following:
①The hydride generation-atomic fluorescence spectrometry (HG-AFS) for mercury analysis established by our group is suits for mercury analysis in the high salinity sample.
②There are different lithology examples of contents in the salt lake as follows: clay > silt > salt containing mealy sand > arenaceous salt with silt particles > pure salt particles. The results showed that salt minerals does not have significant influence for mercury distribution.
③In the Qarhan global core samples, the content of mercury in the section of 0.00～ -10.04m is high, -10.04～-40.27 m is inhomogeneous, -40.27～-49.65 m is low, and -49.65～-82.64 m shows quickly increase, but -82.64～-103.15 m is in reduce trend.
④The geochemical statistical correlations (r) among THg, TFe and TMn in the vertical distribution global core samples with depth 0.00 ~ -47.07 m in the character of salt mineral deposit type in Qaidam Basin are 0.41 and 0.36, respectively. Those results demonstrate that the effect of TFe and TMn in core samples for THg vertical distribution plays is obverious. However, the geochemical statistical correlations (r) among THg, TFe and TMn in the vertical distribution global core samples with depth -47.07 ~ -103.15 m in the character of clay mineral deposit type in Qaidam Basin are 0.41 and 0.36, respectively, and it demonstrates that the effect of iorn and manganese oxidates existed in clay for the vertical distribution of mercury is minor. For vertical distribution of mercury, generally, the effect of iorn oxidates existed core samples between 0.00 and -103.15 m is higher that that of manganese oxidates.
⑤The concentrations of different mercury species in the core of the salt lake is in the order of Hg(oxal) > Hg (pyrite) > Hg(H2O) > Hg(H2O2). it explains that the two main mercury speciations are Hg(oxal) and Hg (pyrite),and the concentrations of dissolved mercery and organic mercury existed in core samples are in minor levels.
主要研究内容:①建立适用于测定盐湖地芯样品及盐湖区内高矿化度水体中汞含量的分析方法;②通过对地芯样品中的总汞(THg)、总铁(TFe)、总锰(TMn)的提取、测定及分析,揭示地芯样品中汞的垂向分布特征;③通过对地芯样品中水溶态汞(Hg-H2O)、铁锰氧化物结合态汞(Hg-oxal)、有机物结合态汞(Hg-H2O2)、硫化矿物吸附态汞(Hg-pyrite)的连续浸提与测定分析,揭示各种形态汞在岩芯样品中的垂向分布与迁移转化规律。
主要研究成果:
①通过改进氢化物发生-原子荧光法(HG-AFS)天然水体系痕量汞分析,建立了可适用于高盐度沉积物样品中汞含量的测定方法;
②察尔汗盐湖不同岩性样品中,总汞(THg)的含量大小为:黏土>淤泥>盐类物质夹粉砂>细纱质盐类>纯石盐,但研究发现,盐类物质对汞的富集作用没有特别明显的差异;
③盐湖地芯样品0 ~ -103.15 m中总汞(THg)含量的垂向分布特征为:总汞的含量由上至下呈表层(0.00 ~ -10.04 m)较高,中间区段(-10.04 ~ -40.27 m)不均一,-40.27 ~-49.65 m较低,-49.65 ~ -82.64 m增大,-82.64 ~ -103.15 m整体含量有所降低的趋势;
④察尔汗盐湖盐类矿物沉积层(0.00 m～-47.07 m)地芯样品中,THg与TFe、TMn的地球化学相关系数分别为0.41和0.36,说明在盐湖沉积层中TFe、TMn对THg的垂向含量分布具有明显影响;在湖相粉砂沉积层(-47.07 m～-103.15 m)地芯样品中,TFe、TMn对THg的地球化学相关系数分别为0.25和0.05,表明湖相沉积层铁锰氧化物对THg的垂向分布影响相对较小。总体而言,在0.00 ~-103.15 m的地芯样品中,含铁氧化物对总汞含量分布的影响大于锰氧化物对总汞分布的影响。
⑤察尔汗盐湖地芯样品中痕量汞各赋存形态的含量大小:Hg(oxal) > Hg (pyrite) > Hg(H_2O) > Hg(H_2O_2) ,说明样品中的汞主要以铁锰氧化物结合态Hg(oxal)和硫化物结合态Hg (pyrite)形式存在;水溶态汞Hg(H_2O)和有机物结合态汞Hg(H_2O_2)在地芯样品中含量极低。
Qarhan Salt Lake located in the central Qaidam Basin is the largest salt lake in China, and it has various mineral in salt lake. The vertical distribution of mercury records the earth's geological information in Qaidam Basin. It would not only demonstrate traces back on the region’s history for mercury migration, but also reflect the geological processing and fluctuation in the palaeoclimate information. The results could reveal the effect of the earth recycling, ecological and the environmental evaluation. Under the joint financial supports from the National Natural Science Foundation of China (Grants 20836009 and 40773045), the vertical distributions of mercury in Qarhan Salt Lake was carried out.
The researching contents include:①Establish a sensitive mercury analysis method for high saline brines and core samples from the salt lake;②The core example includes (expressed as THg), total iron(expressed as TFe), total manganese(expressed as TMn), were extracted determined and then were analyzed. It reveal the vertical distribution of the THg, TFe and TMn.③The Hg-H2O,Hg-oxal,Hg-H2O2 and Hg-pyrite in core samples from the salt lake, were extrated determined and then were analyzed and it reveals the various forms of mercury in the core samples in the vertical distribution and the migation regular pattern.
Solutions in this study can be summerized as following:
①The hydride generation-atomic fluorescence spectrometry (HG-AFS) for mercury analysis established by our group is suits for mercury analysis in the high salinity sample.
②There are different lithology examples of contents in the salt lake as follows: clay > silt > salt containing mealy sand > arenaceous salt with silt particles > pure salt particles. The results showed that salt minerals does not have significant influence for mercury distribution.
③In the Qarhan global core samples, the content of mercury in the section of 0.00～ -10.04m is high, -10.04～-40.27 m is inhomogeneous, -40.27～-49.65 m is low, and -49.65～-82.64 m shows quickly increase, but -82.64～-103.15 m is in reduce trend.
④The geochemical statistical correlations (r) among THg, TFe and TMn in the vertical distribution global core samples with depth 0.00 ~ -47.07 m in the character of salt mineral deposit type in Qaidam Basin are 0.41 and 0.36, respectively. Those results demonstrate that the effect of TFe and TMn in core samples for THg vertical distribution plays is obverious. However, the geochemical statistical correlations (r) among THg, TFe and TMn in the vertical distribution global core samples with depth -47.07 ~ -103.15 m in the character of clay mineral deposit type in Qaidam Basin are 0.41 and 0.36, respectively, and it demonstrates that the effect of iorn and manganese oxidates existed in clay for the vertical distribution of mercury is minor. For vertical distribution of mercury, generally, the effect of iorn oxidates existed core samples between 0.00 and -103.15 m is higher that that of manganese oxidates.
⑤The concentrations of different mercury species in the core of the salt lake is in the order of Hg(oxal) > Hg (pyrite) > Hg(H2O) > Hg(H2O2). it explains that the two main mercury speciations are Hg(oxal) and Hg (pyrite),and the concentrations of dissolved mercery and organic mercury existed in core samples are in minor levels.
引文
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