Identification of multiple mercury sources to stream sediments near Oak Ridge, TN, USA

Donovan, Patrick M.; Blum, Joel D.; Demers, Jason D.; Gu, Baohua; Brooks, Scott C.; Peryam, John

doi:10.1021/es4046549

Title: Identification of multiple mercury sources to stream sediments near Oak Ridge, TN, USA

Abstract

In this paper, sediments were analyzed for total Hg concentration (THg) and isotopic composition from streams and rivers in the vicinity of the Y-12 National Security Complex (Y12) in Oak Ridge, TN (USA). In the stream directly draining Y12, where industrial releases of mercury (Hg) have been documented, high THg (3.26 to 60.1 μg/g) sediments had a distinct Hg isotopic composition (δ²⁰²Hg of 0.02 ± 0.15‰ and Δ¹⁹⁹Hg of -0.07 ± 0.03‰; mean ± 1SD, n=12) compared to sediments from relatively uncontaminated streams in the region (δ²⁰²Hg = -1.40 ± 0.06‰ and Δ¹⁹⁹Hg of –0.26 ± 0.03‰; mean ± 1SD, n=6). Additionally, several streams that are nearby but do not drain Y12 had sediments with intermediate THg (0.06 to 0.21 μg/g) and anomalous δ²⁰²Hg (as low as -5.07‰). We suggest that the low δ²⁰²Hg values in these sediments provide evidence for the contribution of an additional Hg source to sediments, possibly derived from atmospheric deposition. In sediments directly downstream of Y12 this third Hg source is not discernible and the Hg isotopic composition can be largely explained by the mixing of low THg sediments with high THg sediments contaminated by Y12 discharges.

Authors:

Donovan, Patrick M. ^[1]; Blum, Joel D. ^[1]; Demers, Jason D. ^[1]; Gu, Baohua ^[2]; Brooks, Scott C. ^[2]; Peryam, John ^[3]

Univ. of Michigan, Ann Arbor, MI (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Tennessee Department of Environment and Conservation, Oak Ridge, TN (United States)

Publication Date:: Mon Mar 03 00:00:00 EST 2014

Research Org.:: Univ. of Michigan, Ann Arbor, MI (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Biological and Environmental Research (BER)

OSTI Identifier:: 1239629

Grant/Contract Number:: SC0007042

Resource Type:: Accepted Manuscript

Journal Name:: Environmental Science and Technology

Additional Journal Information:: Journal Volume: 48; Journal Issue: 7; Journal ID: ISSN 0013-936X

Publisher:: American Chemical Society (ACS)

Country of Publication:: United States

Language:: English

Subject:: 54 ENVIRONMENTAL SCIENCES; mercury isotopes; river sediments; East Fork Poplar Creek; Clinch River

Citation Formats


                    Donovan, Patrick M., Blum, Joel D., Demers, Jason D., Gu, Baohua, Brooks, Scott C., and Peryam, John. Identification of multiple mercury sources to stream sediments near Oak Ridge, TN, USA.  United States: N. p., 2014. 
Web.  doi:10.1021/es4046549.

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                    Donovan, Patrick M., Blum, Joel D., Demers, Jason D., Gu, Baohua, Brooks, Scott C., & Peryam, John. Identification of multiple mercury sources to stream sediments near Oak Ridge, TN, USA.  United States.  https://doi.org/10.1021/es4046549

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                    Donovan, Patrick M., Blum, Joel D., Demers, Jason D., Gu, Baohua, Brooks, Scott C., and Peryam, John. Mon .  
"Identification of multiple mercury sources to stream sediments near Oak Ridge, TN, USA".  United States.  https://doi.org/10.1021/es4046549.  https://www.osti.gov/servlets/purl/1239629.

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@article{osti_1239629,

  title        = {Identification of multiple mercury sources to stream sediments near Oak Ridge, TN, USA},

  author       = {Donovan, Patrick M. and Blum, Joel D. and Demers, Jason D. and Gu, Baohua and Brooks, Scott C. and Peryam, John},

  abstractNote = {In this paper, sediments were analyzed for total Hg concentration (THg) and isotopic composition from streams and rivers in the vicinity of the Y-12 National Security Complex (Y12) in Oak Ridge, TN (USA). In the stream directly draining Y12, where industrial releases of mercury (Hg) have been documented, high THg (3.26 to 60.1 μg/g) sediments had a distinct Hg isotopic composition (δ202Hg of 0.02 ± 0.15‰ and Δ199Hg of -0.07 ± 0.03‰; mean ± 1SD, n=12) compared to sediments from relatively uncontaminated streams in the region (δ202Hg = -1.40 ± 0.06‰ and Δ199Hg of –0.26 ± 0.03‰; mean ± 1SD, n=6). Additionally, several streams that are nearby but do not drain Y12 had sediments with intermediate THg (0.06 to 0.21 μg/g) and anomalous δ202Hg (as low as -5.07‰). We suggest that the low δ202Hg values in these sediments provide evidence for the contribution of an additional Hg source to sediments, possibly derived from atmospheric deposition. In sediments directly downstream of Y12 this third Hg source is not discernible and the Hg isotopic composition can be largely explained by the mixing of low THg sediments with high THg sediments contaminated by Y12 discharges.},

  doi          = {10.1021/es4046549},

  journal      = {Environmental Science and Technology},

  number       = 7,

  volume       = 48,

  place        = {United States},

  year         = {Mon Mar 03 00:00:00 EST 2014},

  month        = {Mon Mar 03 00:00:00 EST 2014}

}

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Title: Identification of multiple mercury sources to stream sediments near Oak Ridge, TN, USA

Abstract

Citation Formats

Mercury Distribution Across 14 U.S. Forests. Part I: Spatial Patterns of Concentrations in Biomass, Litter, and Soils journal, May 2011

Mercury isotopes in a forested ecosystem: Implications for air-surface exchange dynamics and the global mercury cycle: MERCURY ISOTOPES IN A FORESTED ECOSYSTEM journal, March 2013

Sources of mercury to San Francisco Bay surface sediment as revealed by mercury stable isotopes journal, February 2011

Microbial stable isotope fractionation of mercury: A synthesis of present understanding and future directions journal, January 2013

Mercury isotope fractionation during volatilization of Hg(0) from solution into the gas phase journal, January 2007

Mercury stable isotopes in sediments and largemouth bass from Florida lakes, USA journal, March 2013

Investigation of Local Mercury Deposition from a Coal-Fired Power Plant Using Mercury Isotopes journal, November 2011

Equilibrium Mercury Isotope Fractionation between Dissolved Hg(II) Species and Thiol-Bound Hg journal, June 2010

Mercury isotope fractionation during photoreduction in natural water is controlled by its Hg/DOC ratio journal, November 2009

Mercury concentrations and mercury isotope composition in lake sediment cores from the vicinity of a metal smelting facility in Flin Flon, Manitoba journal, January 2013

Mercury distributions and mercury isotope signatures in sediments of Dongjiang, the Pearl River Delta, China journal, August 2011

Sedimentary mercury stable isotope records of atmospheric and riverine pollution from two major European heavy metal refineries journal, December 2010

Reporting of variations in the natural isotopic composition of mercury journal, March 2007

Use and Legacy of Mercury in the Andes journal, April 2013

Natural Mercury Isotope Variation in Coal Deposits and Organic Soils journal, November 2008

Hg Speciation and Stable Isotope Signatures in Human Hair As a Tracer for Dietary and Occupational Exposure to Mercury journal, December 2011

Mercury distribution and speciation in floodplain soils and uptake into native earthworms (Diplocardia spp.) journal, January 2012

Binding, distribution, and plant uptake of mercury in a soil from Oak Ridge, Tennessee, USA journal, September 2006

Decreasing aqueous mercury concentrations to meet the water quality criterion in fish: Examining the water–fish relationship in two point-source contaminated streams journal, January 2013

Indirect gold trap–MC-ICP-MS coupling for Hg stable isotope analysis using a syringe injection interface journal, January 2008

Characterization of soils from an industrial complex contaminated with elemental mercury journal, August 2013

Mercury distribution in poplar creek, Oak Ridge, Tennessee, USA journal, July 1998

Simulation of flow and mercury transport in Upper East Fork Poplar Creek, Oak Ridge, Tennessee: Simulation of Flow and Mercury Transport in Upper East Fork Poplar Creek, Oak Ridge, Tennessee journal, March 2012

Environmental Impacts of the Tennessee Valley Authority Kingston Coal Ash Spill. 1. Source Apportionment Using Mercury Stable Isotopes journal, December 2012

Tracing Mercury Contamination from the Idrija Mining Region (Slovenia) to the Gulf of Trieste Using Hg Isotope Ratio Measurements journal, January 2009

Mass-Dependent and -Independent Fractionation of Hg Isotopes by Photoreduction in Aquatic Systems journal, October 2007

Identification of contamination in a lake sediment core using Hg and Pb isotopic compositions, Lake Ballinger, Washington, USA journal, February 2013

Mercury characterization in a soil sample collected nearby the DOE Oak Ridge Reservation utilizing sequential extraction and thermal desorption method journal, October 2006

Global Biogeochemical Cycling of Mercury: A Review journal, November 2009

History of mercury use and environmental contamination at the Oak Ridge Y-12 Plant journal, January 2011

Twenty-Five Years of Ecological Recovery of East Fork Poplar Creek: Review of Environmental Problems and Remedial Actions journal, March 2011

Mercury isotope fractionation during liquid–vapor evaporation experiments journal, May 2009

Sources of mercury in a contaminated stream-implications for the timescale of recovery journal, February 2013

Sources and Transfers of Methylmercury in Adjacent River and Forest Food Webs journal, October 2012

Mercury Stable Isotope Fractionation during Reduction of Hg(II) by Different Microbial Pathways journal, December 2008

Isotopic Variability of Mercury in Ore, Mine-Waste Calcine, and Leachates of Mine-Waste Calcine from Areas Mined for Mercury journal, August 2009

Mercury stable isotope fractionation in six utility boilers of two large coal-fired power plants journal, January 2013

Micrometeorological Gradient Approach for Quantifying Air/Surface Exchange of Mercury Vapor: Tests Over Contaminated Soils journal, January 1995

Tracing Sources and Bioaccumulation of Mercury in Fish of Lake Baikal− Angara River Using Hg Isotopic Composition journal, November 2010

Mercury isotope fractionation in waters and sediments of the Murray Brook mine watershed (New Brunswick, Canada): Tracing mercury contamination and transformation journal, January 2013

An isotopic record of mercury in San Francisco Bay sediment journal, June 2013

Species-Specific Stable Isotope Fractionation of Mercury during Hg(II) Methylation by an Anaerobic Bacteria ( Desulfobulbus propionicus ) under Dark Conditions journal, December 2009

Atmospheric concentrations and deposition of Hg to A deciduous forest atwalker branch watershed, Tennessee, USA journal, April 1991

Formation of Mercuric Sulfide in Soil journal, November 1997

Isotopic Composition and Fractionation of Mercury in Great Lakes Precipitation and Ambient Air journal, October 2010

Mercury Isotopes Link Mercury in San Francisco Bay Forage Fish to Surface Sediments journal, February 2011

Mass-dependent and mass-independent variations in the isotope composition of mercury in cores from lakes polluted by a smelter: Effects of smelter emissions, natural processes, and their interactions journal, August 2013

Stable Mercury Isotope Variation in Rice Plants (Oryza sativa L.) from the Wanshan Mercury Mining District, SW China journal, February 2013

Mercury contamination in the riparian zones along the East Fork Poplar Creek at Oak Ridge journal, March 2011

Mercury speciation and mercury isotope fractionation during ore roasting process and their implication to source identification of downstream sediment in the Wanshan mercury mining area, SW China journal, January 2013

Mercury Isotopic Evidence for Multiple Mercury Sources in Coal from the Illinois Basin journal, February 2011

Extractability and Bioavailability of Mercury from a Mercury Sulfide Contaminated Soil in Oak Ridge, Tennessee, USA journal, April 2008

Solution Speciation Controls Mercury Isotope Fractionation of Hg(II) Sorption to Goethite journal, May 2012

Hg isotopes reveal in-stream processing and legacy inputs in East Fork Poplar Creek, Oak Ridge, Tennessee, USA journal, January 2018

A model of mercury cycling and isotopic fractionation in the ocean journal, January 2018

Mercury Accumulation in Tree Rings: Observed Trends in Quantity and Isotopic Composition in Shenandoah National Park, Virginia journal, February 2020

Fate of mercury from artisanal and small-scale gold mining in tropical rivers: Hydrological and biogeochemical controls. A critical review journal, July 2019

Mercury Distribution Across 14 U.S. Forests. Part I: Spatial Patterns of Concentrations in Biomass, Litter, and Soils
journal, May 2011

Mercury isotopes in a forested ecosystem: Implications for air-surface exchange dynamics and the global mercury cycle: MERCURY ISOTOPES IN A FORESTED ECOSYSTEM
journal, March 2013

Sources of mercury to San Francisco Bay surface sediment as revealed by mercury stable isotopes
journal, February 2011

Microbial stable isotope fractionation of mercury: A synthesis of present understanding and future directions
journal, January 2013

Mercury isotope fractionation during volatilization of Hg(0) from solution into the gas phase
journal, January 2007

Mercury stable isotopes in sediments and largemouth bass from Florida lakes, USA
journal, March 2013

Investigation of Local Mercury Deposition from a Coal-Fired Power Plant Using Mercury Isotopes
journal, November 2011

Equilibrium Mercury Isotope Fractionation between Dissolved Hg(II) Species and Thiol-Bound Hg
journal, June 2010

Mercury isotope fractionation during photoreduction in natural water is controlled by its Hg/DOC ratio
journal, November 2009

Mercury concentrations and mercury isotope composition in lake sediment cores from the vicinity of a metal smelting facility in Flin Flon, Manitoba
journal, January 2013

Mercury distributions and mercury isotope signatures in sediments of Dongjiang, the Pearl River Delta, China
journal, August 2011

Sedimentary mercury stable isotope records of atmospheric and riverine pollution from two major European heavy metal refineries
journal, December 2010

Reporting of variations in the natural isotopic composition of mercury
journal, March 2007

Use and Legacy of Mercury in the Andes
journal, April 2013

Natural Mercury Isotope Variation in Coal Deposits and Organic Soils
journal, November 2008

Hg Speciation and Stable Isotope Signatures in Human Hair As a Tracer for Dietary and Occupational Exposure to Mercury
journal, December 2011

Mercury distribution and speciation in floodplain soils and uptake into native earthworms (Diplocardia spp.)
journal, January 2012

Binding, distribution, and plant uptake of mercury in a soil from Oak Ridge, Tennessee, USA
journal, September 2006

Decreasing aqueous mercury concentrations to meet the water quality criterion in fish: Examining the water–fish relationship in two point-source contaminated streams
journal, January 2013

Indirect gold trap–MC-ICP-MS coupling for Hg stable isotope analysis using a syringe injection interface
journal, January 2008

Characterization of soils from an industrial complex contaminated with elemental mercury
journal, August 2013

Mercury distribution in poplar creek, Oak Ridge, Tennessee, USA
journal, July 1998

Simulation of flow and mercury transport in Upper East Fork Poplar Creek, Oak Ridge, Tennessee: Simulation of Flow and Mercury Transport in Upper East Fork Poplar Creek, Oak Ridge, Tennessee
journal, March 2012

Environmental Impacts of the Tennessee Valley Authority Kingston Coal Ash Spill. 1. Source Apportionment Using Mercury Stable Isotopes
journal, December 2012

Tracing Mercury Contamination from the Idrija Mining Region (Slovenia) to the Gulf of Trieste Using Hg Isotope Ratio Measurements
journal, January 2009

Mass-Dependent and -Independent Fractionation of Hg Isotopes by Photoreduction in Aquatic Systems
journal, October 2007

Identification of contamination in a lake sediment core using Hg and Pb isotopic compositions, Lake Ballinger, Washington, USA
journal, February 2013

Mercury characterization in a soil sample collected nearby the DOE Oak Ridge Reservation utilizing sequential extraction and thermal desorption method
journal, October 2006

Global Biogeochemical Cycling of Mercury: A Review
journal, November 2009

History of mercury use and environmental contamination at the Oak Ridge Y-12 Plant
journal, January 2011

Twenty-Five Years of Ecological Recovery of East Fork Poplar Creek: Review of Environmental Problems and Remedial Actions
journal, March 2011

Mercury isotope fractionation during liquid–vapor evaporation experiments
journal, May 2009

Sources of mercury in a contaminated stream-implications for the timescale of recovery
journal, February 2013

Sources and Transfers of Methylmercury in Adjacent River and Forest Food Webs
journal, October 2012

Mercury Stable Isotope Fractionation during Reduction of Hg(II) by Different Microbial Pathways
journal, December 2008

Isotopic Variability of Mercury in Ore, Mine-Waste Calcine, and Leachates of Mine-Waste Calcine from Areas Mined for Mercury
journal, August 2009

Mercury stable isotope fractionation in six utility boilers of two large coal-fired power plants
journal, January 2013

Micrometeorological Gradient Approach for Quantifying Air/Surface Exchange of Mercury Vapor: Tests Over Contaminated Soils
journal, January 1995

Tracing Sources and Bioaccumulation of Mercury in Fish of Lake Baikal− Angara River Using Hg Isotopic Composition
journal, November 2010

Mercury isotope fractionation in waters and sediments of the Murray Brook mine watershed (New Brunswick, Canada): Tracing mercury contamination and transformation
journal, January 2013

An isotopic record of mercury in San Francisco Bay sediment
journal, June 2013

Species-Specific Stable Isotope Fractionation of Mercury during Hg(II) Methylation by an Anaerobic Bacteria ( Desulfobulbus propionicus ) under Dark Conditions
journal, December 2009

Atmospheric concentrations and deposition of Hg to A deciduous forest atwalker branch watershed, Tennessee, USA
journal, April 1991

Formation of Mercuric Sulfide in Soil
journal, November 1997

Isotopic Composition and Fractionation of Mercury in Great Lakes Precipitation and Ambient Air
journal, October 2010

Mercury Isotopes Link Mercury in San Francisco Bay Forage Fish to Surface Sediments
journal, February 2011

Mass-dependent and mass-independent variations in the isotope composition of mercury in cores from lakes polluted by a smelter: Effects of smelter emissions, natural processes, and their interactions
journal, August 2013

Stable Mercury Isotope Variation in Rice Plants (Oryza sativa L.) from the Wanshan Mercury Mining District, SW China
journal, February 2013

Mercury contamination in the riparian zones along the East Fork Poplar Creek at Oak Ridge
journal, March 2011

Mercury speciation and mercury isotope fractionation during ore roasting process and their implication to source identification of downstream sediment in the Wanshan mercury mining area, SW China
journal, January 2013

Mercury Isotopic Evidence for Multiple Mercury Sources in Coal from the Illinois Basin
journal, February 2011

Extractability and Bioavailability of Mercury from a Mercury Sulfide Contaminated Soil in Oak Ridge, Tennessee, USA
journal, April 2008

Solution Speciation Controls Mercury Isotope Fractionation of Hg(II) Sorption to Goethite
journal, May 2012

Hg isotopes reveal in-stream processing and legacy inputs in East Fork Poplar Creek, Oak Ridge, Tennessee, USA
journal, January 2018

A model of mercury cycling and isotopic fractionation in the ocean
journal, January 2018

Mercury Accumulation in Tree Rings: Observed Trends in Quantity and Isotopic Composition in Shenandoah National Park, Virginia
journal, February 2020

Fate of mercury from artisanal and small-scale gold mining in tropical rivers: Hydrological and biogeochemical controls. A critical review
journal, July 2019