Formation of soluble mercury oxide coatings: Transformation of elemental mercury in soils

Miller, Carrie L.; Watson, David B.; Lester, Brian P.; Howe, Jane Y.; Phillips, Debra H.; He, Feng; Liang, Liyuan; Pierce, Eric M.

doi:10.1021/acs.est.5b00263

Title: Formation of soluble mercury oxide coatings: Transformation of elemental mercury in soils

Abstract

In this study, the impact of mercury (Hg) on human and ecological health has been known for decades. Although a treaty signed in 2013 by 147 nations regulates future large-scale mercury emissions, legacy Hg contamination exists worldwide and small-scale releases will continue. The fate of elemental mercury, Hg(0), lost to the subsurface and its potential chemical transformation that can lead to changes in speciation and mobility are poorly understood. Here, we show that Hg(0) beads interact with soil or manganese oxide solids and X-ray spectroscopic analysis indicates that the soluble mercury coatings are HgO. Dissolution studies show that, after reacting with a composite soil, >20 times more Hg is released into water from the coated beads than from a pure liquid mercury bead. An even larger, >700 times, release occurs from coated Hg(0) beads that have been reacted with manganese oxide, suggesting that manganese oxides are involved in the transformation of the Hg(0) beads and creation of the soluble mercury coatings. Although the coatings may inhibit Hg(0) evaporation, the high solubility of the coatings can enhance Hg(II) migration away from the Hg(0)-spill site and result in potential changes in mercury speciation in the soil and increased mercury mobility.

Authors:

Miller, Carrie L. ^[1]; Watson, David B. ^[2]; Lester, Brian P. ^[2]; Howe, Jane Y. ^[3]; Phillips, Debra H. ^[4]; He, Feng ^[5]; Liang, Liyuan ^[2]; Pierce, Eric M. ^[2]

Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Troy Univ., Troy, AL (United States)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Hitachi High Technologies Canada, Inc., Toronto, ON (Canada)
Queen's Univ. Belfast, Belfast (United Kingdom)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Zhejiang Univ. of Technology, Zhejiang (People's Republic of China)

Publication Date:: Mon Sep 21 00:00:00 EDT 2015

Research Org.:: Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

Sponsoring Org.:: USDOE Office of Environmental Management (EM)

OSTI Identifier:: 1255647

Grant/Contract Number:: AC05-00OR22725

Resource Type:: Accepted Manuscript

Journal Name:: Environmental Science and Technology

Additional Journal Information:: Journal Volume: 49; Journal Issue: 20; Journal ID: ISSN 0013-936X

Publisher:: American Chemical Society (ACS)

Country of Publication:: United States

Language:: English

Subject:: 58 GEOSCIENCES

Citation Formats


                    Miller, Carrie L., Watson, David B., Lester, Brian P., Howe, Jane Y., Phillips, Debra H., He, Feng, Liang, Liyuan, and Pierce, Eric M. Formation of soluble mercury oxide coatings: Transformation of elemental mercury in soils.  United States: N. p., 2015. 
Web.  doi:10.1021/acs.est.5b00263.

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                    Miller, Carrie L., Watson, David B., Lester, Brian P., Howe, Jane Y., Phillips, Debra H., He, Feng, Liang, Liyuan, & Pierce, Eric M. Formation of soluble mercury oxide coatings: Transformation of elemental mercury in soils.  United States.  https://doi.org/10.1021/acs.est.5b00263

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                    Miller, Carrie L., Watson, David B., Lester, Brian P., Howe, Jane Y., Phillips, Debra H., He, Feng, Liang, Liyuan, and Pierce, Eric M. Mon .  
"Formation of soluble mercury oxide coatings: Transformation of elemental mercury in soils".  United States.  https://doi.org/10.1021/acs.est.5b00263.  https://www.osti.gov/servlets/purl/1255647.

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@article{osti_1255647,

  title        = {Formation of soluble mercury oxide coatings: Transformation of elemental mercury in soils},

  author       = {Miller, Carrie L. and Watson, David B. and Lester, Brian P. and Howe, Jane Y. and Phillips, Debra H. and He, Feng and Liang, Liyuan and Pierce, Eric M.},

  abstractNote = {In this study, the impact of mercury (Hg) on human and ecological health has been known for decades. Although a treaty signed in 2013 by 147 nations regulates future large-scale mercury emissions, legacy Hg contamination exists worldwide and small-scale releases will continue. The fate of elemental mercury, Hg(0), lost to the subsurface and its potential chemical transformation that can lead to changes in speciation and mobility are poorly understood. Here, we show that Hg(0) beads interact with soil or manganese oxide solids and X-ray spectroscopic analysis indicates that the soluble mercury coatings are HgO. Dissolution studies show that, after reacting with a composite soil, >20 times more Hg is released into water from the coated beads than from a pure liquid mercury bead. An even larger, >700 times, release occurs from coated Hg(0) beads that have been reacted with manganese oxide, suggesting that manganese oxides are involved in the transformation of the Hg(0) beads and creation of the soluble mercury coatings. Although the coatings may inhibit Hg(0) evaporation, the high solubility of the coatings can enhance Hg(II) migration away from the Hg(0)-spill site and result in potential changes in mercury speciation in the soil and increased mercury mobility.},

  doi          = {10.1021/acs.est.5b00263},

  journal      = {Environmental Science and Technology},

  number       = 20,

  volume       = 49,

  place        = {United States},

  year         = {Mon Sep 21 00:00:00 EDT 2015},

  month        = {Mon Sep 21 00:00:00 EDT 2015}

}

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Works referencing / citing this record:

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

Moreno-Brush, Mónica; McLagan, David S.; Biester, Harald
Critical Reviews in Environmental Science and Technology, Vol. 50, Issue 5
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Title: Formation of soluble mercury oxide coatings: Transformation of elemental mercury in soils

Abstract

Citation Formats

Contribution of contaminated sites to the global mercury budget journal, August 2013

Global Change and Mercury journal, September 2013

Selective extractions to assess the biogeochemically relevant fractionation of inorganic mercury in sediments and soils journal, March 2003

Quantification of mercury in soils and sediments - acid digestion versus pyrolysis journal, June 1997

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Mercury Speciation by X-ray Absorption Fine Structure Spectroscopy and Sequential Chemical Extractions: A Comparison of Speciation Methods journal, November 2003

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Complexation of Mercury(II) in Soil Organic Matter: EXAFS Evidence for Linear Two-Coordination with Reduced Sulfur Groups journal, July 2006

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

Dark Oxidation of Dissolved and Liquid Elemental Mercury in Aquatic Environments journal, January 2005

Arsenic Adsorption and Oxidation at Manganite Surfaces. 1. Method for Simultaneous Determination of Adsorbed and Dissolved Arsenic Species journal, May 2000

Chromium(III) oxidation by .delta.-manganese oxide (MnO2). 1. Characterization journal, January 1992

Oxidation of Chromium(III) to (VI) by Manganese Oxides journal, January 2002

Reduction and Oxidation Processes of Chromium in Soils journal, January 2000

Structural mechanism of Co (super 2+) oxidation by the phyllomanganate buserite journal, December 1997

Oxidative power of Mn(IV) and Fe(III) oxides with respect to As(III) in terrestrial and aquatic environments journal, May 1981

Manganese oxide minerals: Crystal structures and economic and environmental significance journal, March 1999

Spectroscopic Study of Surface Redox Reactions with Manganese Oxides journal, January 1992

The effects of MnO2 on sorption and oxidation of Cr(III) by soils journal, October 2004

Uraninite oxidation and dissolution induced by manganese oxide: A redox reaction between two insoluble minerals journal, January 2013

Uranium Deposition in a Weathered Fractured Saprolite/Shale journal, November 2007

Possible mechanism of elemental mercury oxidation in the presence of sh compounds in aqueous solution journal, July 1995

Stimulation of elemental mercury oxidation in the presence of chloride ion in aquatic environments journal, March 1996

Simulation of the Chemical Fate and Bioavailability of Liquid Elemental Mercury Drops from Gold Mining in Amazonian Freshwater Systems journal, November 2007

Mercury adsorption and oxidation in coal combustion and gasification processes journal, February 2012

Catalytic Oxidation of Elemental Mercury over the Modified Catalyst Mn/α-Al 2 O 3 at Lower Temperatures journal, December 2009

Adsorption and Catalytic Oxidation of Gaseous Elemental Mercury in Flue Gas over MnO x /Alumina journal, February 2009

Catalytic oxidation of Hg0 by CuO–MnO2–Fe2O3/γ-Al2O3 catalyst journal, June 2013

Mercury as a Global Pollutant: Sources, Pathways, and Effects journal, May 2013

Photooxidation of Hg(0) in Artificial and Natural Waters journal, April 2001

Photoinduced Oxidation of Hg 0 (aq) in the Waters from the St. Lawrence Estuary journal, January 2004

Review Selected properties of simple amalgams journal, August 1989

Kinetics of the reduction of Mn2+ at the dropping mercury electrode journal, November 1967

Mercury speciation in tailings of the Idrija mercury mine journal, May 1999

Soil Remediation – Mercury Speciation in Soil and Vapor Phase During Thermal Treatment journal, April 2008

On the mechanisms of dissolution of montroydite [HgO(s)]: Dependence of the dissolution rate on pH, temperature, and stirring rate journal, May 2006

The distribution of mercury around the small-scale gold mining area along the Cikaniki river, Bogor, Indonesia journal, August 2013

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Distribuição e especiação de mercúrio em sedimentos de áreas de garimpo de ouro do quadrilátero ferrífero (MG) journal, January 2007

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

Contribution of contaminated sites to the global mercury budget
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Global Change and Mercury
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Selective extractions to assess the biogeochemically relevant fractionation of inorganic mercury in sediments and soils
journal, March 2003

Quantification of mercury in soils and sediments - acid digestion versus pyrolysis
journal, June 1997

Mercury speciation analyses in HgCl2-contaminated soils and groundwater—Implications for risk assessment and remediation strategies
journal, January 2008

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

Mercury fractionation in contaminated soils from the Idrija mercury mine region
journal, January 2004

Mercury Speciation by X-ray Absorption Fine Structure Spectroscopy and Sequential Chemical Extractions: A Comparison of Speciation Methods
journal, November 2003

Geological and anthropogenic factors influencing mercury speciation in mine wastes: an EXAFS spectroscopy study
journal, March 2004

Complexation of Mercury(II) in Soil Organic Matter: EXAFS Evidence for Linear Two-Coordination with Reduced Sulfur Groups
journal, July 2006

Mercury speciation in a tropical soil association; Consequence of gold mining on Hg distribution in French Guiana
journal, November 2009

Mercury conversion processes in Amazon soils evaluated by thermodesorption analysis
journal, December 2006

Accumulation and oxidation of elemental mercury in tropical soils
journal, September 2015

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

Dark Oxidation of Dissolved and Liquid Elemental Mercury in Aquatic Environments
journal, January 2005

Arsenic Adsorption and Oxidation at Manganite Surfaces. 1. Method for Simultaneous Determination of Adsorbed and Dissolved Arsenic Species
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Chromium(III) oxidation by .delta.-manganese oxide (MnO2). 1. Characterization
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Oxidation of Chromium(III) to (VI) by Manganese Oxides
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journal, November 2007

Possible mechanism of elemental mercury oxidation in the presence of sh compounds in aqueous solution
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Stimulation of elemental mercury oxidation in the presence of chloride ion in aquatic environments
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Simulation of the Chemical Fate and Bioavailability of Liquid Elemental Mercury Drops from Gold Mining in Amazonian Freshwater Systems
journal, November 2007

Mercury adsorption and oxidation in coal combustion and gasification processes
journal, February 2012

Catalytic Oxidation of Elemental Mercury over the Modified Catalyst Mn/α-Al ₂ O ₃ at Lower Temperatures
journal, December 2009

Adsorption and Catalytic Oxidation of Gaseous Elemental Mercury in Flue Gas over MnO _x /Alumina
journal, February 2009

Catalytic oxidation of Hg0 by CuO–MnO2–Fe2O3/γ-Al2O3 catalyst
journal, June 2013

Mercury as a Global Pollutant: Sources, Pathways, and Effects
journal, May 2013

Photooxidation of Hg(0) in Artificial and Natural Waters
journal, April 2001

Photoinduced Oxidation of Hg ⁰ (aq) in the Waters from the St. Lawrence Estuary
journal, January 2004

Review Selected properties of simple amalgams
journal, August 1989

Kinetics of the reduction of Mn2+ at the dropping mercury electrode
journal, November 1967

Mercury speciation in tailings of the Idrija mercury mine
journal, May 1999

Soil Remediation – Mercury Speciation in Soil and Vapor Phase During Thermal Treatment
journal, April 2008

On the mechanisms of dissolution of montroydite [HgO(s)]: Dependence of the dissolution rate on pH, temperature, and stirring rate
journal, May 2006

The distribution of mercury around the small-scale gold mining area along the Cikaniki river, Bogor, Indonesia
journal, August 2013

The redox processes in Hg-contaminated soils from Descoberto (Minas Gerais, Brazil): Implications for the mercury cycle
journal, February 2015

Distribuição e especiação de mercúrio em sedimentos de áreas de garimpo de ouro do quadrilátero ferrífero (MG)
journal, January 2007

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