Isotopic evidence for distinct sources of mercury in lake waters and sediments

Lakes are important ecosystems where mercury (Hg) may undergo extensive methylation and bioaccumulation in the aquatic food web. It is thus crucial to understand the sources of Hg in lake systems. Mercury isotope composition is a powerful tracer of its sources in the environment. However, previous s...

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Published inChemical geology Vol. 426; pp. 33 - 44
Main Authors Chen, Jiubin, Hintelmann, Holger, Zheng, Wang, Feng, Xinbin, Cai, Hongming, Wang, Zhuhong, Yuan, Shengliu, Wang, Zhongwei
Format Journal Article
LanguageEnglish
Published Elsevier B.V 15.05.2016
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Abstract Lakes are important ecosystems where mercury (Hg) may undergo extensive methylation and bioaccumulation in the aquatic food web. It is thus crucial to understand the sources of Hg in lake systems. Mercury isotope composition is a powerful tracer of its sources in the environment. However, previous studies on Hg isotope compositions in lake systems mainly focus on the aquatic organism and sediments, whereas lake water that provides the nutrients for the bottom of aquatic food chain has received much less attention. Here we report Hg isotope compositions in surface water and sediments of 8 freshwater lakes in Ontario, Canada. We determined significantly positive Δ199Hg and Δ200Hg values in surface water of all lakes, which are similar to previously reported isotope signature of local atmospheric precipitation. In contrast, the isotope compositions of lake sediments show predominantly negative Δ199Hg and negligible Δ200Hg values that are similar to atmospheric elemental Hg(0) and terrestrial soils and plants. We conclude that the source of Hg in lake surface water is likely dominated by direct atmospheric precipitation, while the Hg in lake sediments is primarily derived from watershed inputs of terrestrial particles. The concurrent odd Hg isotope anomalies in surface waters suggest that methylmercury (MeHg) from the watershed wetland, together with Hg(II) derived from the catchment weathering is likely another Hg source to lake waters besides atmospheric deposition. We suggest that the different Hg sources and isotope compositions between lake water and sediments would result in different isotope signatures for MeHg that is produced in water column and in sediments. Therefore, our study not only elucidates the sources of Hg to lake systems, but also has implications in distinguishing between different MeHg sources and in tracing the bioaccumulation of MeHg in aquatic organism. •Occurrence of even mercury isotope anomalies is imprinted onto surface water.•Mercury isotope anomalies establish a direct link of Hg in lake surface waters to atmospheric deposition.•Watershed methylmercury is also an important Hg source in lake waters and food webs.•Lake sediments are isotopically decoupled from the lake waters and the atmosphere.
AbstractList Lakes are important ecosystems where mercury (Hg) may undergo extensive methylation and bioaccumulation in the aquatic food web. It is thus crucial to understand the sources of Hg in lake systems. Mercury isotope composition is a powerful tracer of its sources in the environment. However, previous studies on Hg isotope compositions in lake systems mainly focus on the aquatic organism and sediments, whereas lake water that provides the nutrients for the bottom of aquatic food chain has received much less attention. Here we report Hg isotope compositions in surface water and sediments of 8 freshwater lakes in Ontario, Canada. We determined significantly positive Delta 199Hg and Delta 200Hg values in surface water of all lakes, which are similar to previously reported isotope signature of local atmospheric precipitation. In contrast, the isotope compositions of lake sediments show predominantly negative Delta 199Hg and negligible Delta 200Hg values that are similar to atmospheric elemental Hg(0) and terrestrial soils and plants. We conclude that the source of Hg in lake surface water is likely dominated by direct atmospheric precipitation, while the Hg in lake sediments is primarily derived from watershed inputs of terrestrial particles. The concurrent odd Hg isotope anomalies in surface waters suggest that methylmercury (MeHg) from the watershed wetland, together with Hg(II) derived from the catchment weathering is likely another Hg source to lake waters besides atmospheric deposition. We suggest that the different Hg sources and isotope compositions between lake water and sediments would result in different isotope signatures for MeHg that is produced in water column and in sediments. Therefore, our study not only elucidates the sources of Hg to lake systems, but also has implications in distinguishing between different MeHg sources and in tracing the bioaccumulation of MeHg in aquatic organism.
Lakes are important ecosystems where mercury (Hg) may undergo extensive methylation and bioaccumulation in the aquatic food web. It is thus crucial to understand the sources of Hg in lake systems. Mercury isotope composition is a powerful tracer of its sources in the environment. However, previous studies on Hg isotope compositions in lake systems mainly focus on the aquatic organism and sediments, whereas lake water that provides the nutrients for the bottom of aquatic food chain has received much less attention. Here we report Hg isotope compositions in surface water and sediments of 8 freshwater lakes in Ontario, Canada. We determined significantly positive Δ199Hg and Δ200Hg values in surface water of all lakes, which are similar to previously reported isotope signature of local atmospheric precipitation. In contrast, the isotope compositions of lake sediments show predominantly negative Δ199Hg and negligible Δ200Hg values that are similar to atmospheric elemental Hg(0) and terrestrial soils and plants. We conclude that the source of Hg in lake surface water is likely dominated by direct atmospheric precipitation, while the Hg in lake sediments is primarily derived from watershed inputs of terrestrial particles. The concurrent odd Hg isotope anomalies in surface waters suggest that methylmercury (MeHg) from the watershed wetland, together with Hg(II) derived from the catchment weathering is likely another Hg source to lake waters besides atmospheric deposition. We suggest that the different Hg sources and isotope compositions between lake water and sediments would result in different isotope signatures for MeHg that is produced in water column and in sediments. Therefore, our study not only elucidates the sources of Hg to lake systems, but also has implications in distinguishing between different MeHg sources and in tracing the bioaccumulation of MeHg in aquatic organism. •Occurrence of even mercury isotope anomalies is imprinted onto surface water.•Mercury isotope anomalies establish a direct link of Hg in lake surface waters to atmospheric deposition.•Watershed methylmercury is also an important Hg source in lake waters and food webs.•Lake sediments are isotopically decoupled from the lake waters and the atmosphere.
Author Feng, Xinbin
Cai, Hongming
Zheng, Wang
Hintelmann, Holger
Chen, Jiubin
Wang, Zhuhong
Yuan, Shengliu
Wang, Zhongwei
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  surname: Chen
  fullname: Chen, Jiubin
  email: chenjiubin@vip.gyig.ac.cn
  organization: State Key laboratory of Environmental Geochemistry, Institute of Geochemistry, Chinese Academy of Sciences, 99 Linchengxi Road, Guiyang, GuiZhou 550081, China
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  givenname: Holger
  surname: Hintelmann
  fullname: Hintelmann, Holger
  organization: Chemistry Department, Trent University, 1600 West Bank Drive, Peterborough, Ontario K9J7B8, Canada
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  surname: Zheng
  fullname: Zheng, Wang
  organization: Department of Earth Sciences, University of Toronto, Toronto, ON M5S 3B1, Canada
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  givenname: Xinbin
  surname: Feng
  fullname: Feng, Xinbin
  organization: State Key laboratory of Environmental Geochemistry, Institute of Geochemistry, Chinese Academy of Sciences, 99 Linchengxi Road, Guiyang, GuiZhou 550081, China
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  givenname: Hongming
  surname: Cai
  fullname: Cai, Hongming
  organization: State Key laboratory of Environmental Geochemistry, Institute of Geochemistry, Chinese Academy of Sciences, 99 Linchengxi Road, Guiyang, GuiZhou 550081, China
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  givenname: Zhuhong
  surname: Wang
  fullname: Wang, Zhuhong
  organization: State Key laboratory of Environmental Geochemistry, Institute of Geochemistry, Chinese Academy of Sciences, 99 Linchengxi Road, Guiyang, GuiZhou 550081, China
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  givenname: Shengliu
  surname: Yuan
  fullname: Yuan, Shengliu
  organization: State Key laboratory of Environmental Geochemistry, Institute of Geochemistry, Chinese Academy of Sciences, 99 Linchengxi Road, Guiyang, GuiZhou 550081, China
– sequence: 8
  givenname: Zhongwei
  surname: Wang
  fullname: Wang, Zhongwei
  organization: State Key laboratory of Environmental Geochemistry, Institute of Geochemistry, Chinese Academy of Sciences, 99 Linchengxi Road, Guiyang, GuiZhou 550081, China
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Snippet Lakes are important ecosystems where mercury (Hg) may undergo extensive methylation and bioaccumulation in the aquatic food web. It is thus crucial to...
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SubjectTerms Atmospheric precipitation
Atmospherics
Freshwater
Isotope composition
Isotopes
Lake water and sediments
Lakes
Mass-independent fractionation
Mercury (metal)
Odd and even mercury isotopes
Sediments
Surface water
Watershed input
Watersheds
Title Isotopic evidence for distinct sources of mercury in lake waters and sediments
URI https://dx.doi.org/10.1016/j.chemgeo.2016.01.030
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https://www.proquest.com/docview/1793269157
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