Mobilization of mercury from contaminated creekbank soils

Johs, Alexander; Goñez-Rodríguez, Leroy; Brooks, Scott C.; Mayes, Melanie A.

doi:10.1007/s11368-025-04014-w

Title: Mobilization of mercury from contaminated creekbank soils

Journal Article · Thu May 22 00:00:00 UTC 2025 · Journal of Soils and Sediments

DOI: https://doi.org/10.1007/s11368-025-04014-w · OSTI ID:2573701

^[1]; Goñez-Rodríguez, Leroy ^[1];

^[1];

^[1]

Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

The industrial use of mercury (Hg) led to the contamination of numerous watersheds worldwide, including the East Fork Poplar Creek (EFPC) in Tennessee, USA. Mercury can accumulate in creek banks and floodplain soils and is mobilized into downstream environments due to erosion from precipitation and flooding. Here, this study aimed to evaluate the geochemical conditions contributing to the release of Hg from contaminated soils in this watershed. Bank soil samples from the EFPC watershed with total Hg concentrations ranging from 27.2 to 1,425 mg·kg⁻¹ were used in a series of batch experiments with artificial creek water at a solid-to-solution ratio of 1:30 to assess Hg release. Additional experiments examined Hg release across different soil size fractions and solid-to-solution ratios, as well as the effect of dissolved organic matter and time on Hg mobilization. Mercury release ranged from 0.011 to 0.17% of the total soil Hg and is correlated with total Hg concentrations. Variations in release among size fractions suggested heterogeneous distribution of labile Hg species. Results indicated two distinct solubility regimes depending on solid-to-solution ratios. Dissolved organic matter enhanced Hg release, and time-dependent experiments showed that changes in mercury speciation could decrease dissolved Hg concentrations over time. Identifying conditions that promote Hg mobilization from contaminated soils improves our understanding of Hg fluxes into downstream environments. Key factors influencing mercury release include soil characteristics, water chemistry, and temporal changes in mercury speciation.

View Accepted Manuscript (DOE)

Cite

Export

Save

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Environmental Management (EM)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 2573701

Journal Information:: Journal of Soils and Sediments, Journal Name: Journal of Soils and Sediments Journal Issue: 6 Vol. 25; ISSN 1439-0108; ISSN 1614-7480

Publisher:: Springer NatureCopyright Statement

Country of Publication:: United States

Language:: English

References (46)

Sources of mercury in a contaminated stream-implications for the timescale of recovery Southworth, George; Mathews, Teresa; Greeley, Mark Environmental Toxicology and Chemistry, Vol. 32, Issue 4 https://doi.org/10.1002/Etc.2115	journal	February 2013
The Mercury Problem in Artisanal and Small-Scale Gold Mining Esdaile, Louisa J.; Chalker, Justin M. Chemistry - A European Journal, Vol. 24, Issue 27 https://doi.org/10.1002/chem.201704840	journal	February 2018
Seasonal and flow-driven dynamics of particulate and dissolved mercury and methylmercury in a stream impacted by an industrial mercury source: Hg and MeHg dynamics in an industrially contaminated stream Riscassi, Ami; Miller, Carrie; Brooks, Scott Environmental Toxicology and Chemistry, Vol. 35, Issue 6 https://doi.org/10.1002/etc.3310	journal	March 2016
Die Löslichkeit von Metallsulfiden I. Schwarzes Quecksilbersulfid Schwarzenbach, G.; Widmer, Michael Helvetica Chimica Acta, Vol. 46, Issue 7 https://doi.org/10.1002/hlca.19630460719	journal	January 1963
Characterization of mercury species in contaminated floodplain soils Barnett, M. O.; Harris, L. A.; Turner, R. R. Water, Air, & Soil Pollution, Vol. 80, Issue 1-4 https://doi.org/10.1007/Bf01189771	journal	February 1995
Evaluation of engineered sorbents for the sorption of mercury from contaminated bank soils: a column study Goñez-Rodríguez, Leroy; Johs, Alexander; Lowe, Kenneth A. Environmental Science and Pollution Research, Vol. 28, Issue 18 https://doi.org/10.1007/s11356-020-12073-4	journal	January 2021
Source relationships between streambank soils and streambed sediments in a mercury-contaminated stream Dickson, Johnbull O.; Mayes, Melanie A.; Brooks, Scott C. Journal of Soils and Sediments, Vol. 19, Issue 4 https://doi.org/10.1007/s11368-018-2183-0	journal	November 2018
Investigation of legacy industrial mercury in floodplain soils: South River, Virginia, USA Lazareva, Olesya; Sparks, Donald L.; Landis, Richard Environmental Earth Sciences, Vol. 78, Issue 8 https://doi.org/10.1007/s12665-019-8253-9	journal	April 2019
Oxidative dissolution of metacinnabar (β-HgS) by dissolved oxygen Barnett, Mark O.; Turner, Ralph R.; Singer, Philip C. Applied Geochemistry, Vol. 16, Issue 13 https://doi.org/10.1016/S0883-2927(01)00026-9	journal	October 2001
Mercury mobilization by oxidative dissolution of cinnabar (α-HgS) and metacinnabar (β-HgS) Holley, Elizabeth A.; James McQuillan, A.; Craw, Dave Chemical Geology, Vol. 240, Issue 3-4 https://doi.org/10.1016/j.chemgeo.2007.03.001	journal	June 2007
History of mercury use and environmental contamination at the Oak Ridge Y-12 Plant Brooks, Scott C.; Southworth, George R. Environmental Pollution, Vol. 159, Issue 1 https://doi.org/10.1016/j.envpol.2010.09.009	journal	January 2011
Precipitation of nanoscale mercuric sulfides in the presence of natural organic matter: Structural properties, aggregation, and biotransformation Pham, Anh Le-Tuan; Morris, Amanda; Zhang, Tong Geochimica et Cosmochimica Acta, Vol. 133 https://doi.org/10.1016/j.gca.2014.02.027	journal	May 2014
High methylation potential of mercury complexed with mixed thiolate ligands by Geobacter sulfurreducens PCA Liang, Xujun; Johs, Alexander; Abernathy, Macon J. Geochimica et Cosmochimica Acta, Vol. 342 https://doi.org/10.1016/j.gca.2022.12.008	journal	February 2023
Soil as an archive of coal-fired power plant mercury deposition Rodríguez Martín, José Antonio; Nanos, Nikos Journal of Hazardous Materials, Vol. 308 https://doi.org/10.1016/j.jhazmat.2016.01.026	journal	May 2016
Dissolved organic matter reduces the effectiveness of sorbents for mercury removal Johs, Alexander; Eller, Virginia A.; Mehlhorn, Tonia L. Science of The Total Environment, Vol. 690 https://doi.org/10.1016/j.scitotenv.2019.07.001	journal	November 2019
Influence of Dissolved Organic Matter on the Environmental Fate of Metals, Nanoparticles, and Colloids Aiken, George R.; Hsu-Kim, Heileen; Ryan, Joseph N. Environmental Science & Technology, Vol. 45, Issue 8 https://doi.org/10.1021/Es103992s	journal	April 2011
All-Time Releases of Mercury to the Atmosphere from Human Activities Streets, David G.; Devane, Molly K.; Lu, Zifeng Environmental Science & Technology, Vol. 45, Issue 24 https://doi.org/10.1021/Es202765m	journal	December 2011
Contribution of Coexisting Sulfate and Iron Reducing Bacteria to Methylmercury Production in Freshwater River Sediments Yu, Ri-Qing; Flanders, J. R.; Mack, E. Erin Environmental Science & Technology, Vol. 46, Issue 5, p. 2684-2691 https://doi.org/10.1021/Es2033718	journal	February 2012
Dissolved Organic Matter Enhances Microbial Mercury Methylation Under Sulfidic Conditions Graham, Andrew M.; Aiken, George R.; Gilmour, Cynthia C. Environmental Science & Technology, Vol. 46, Issue 5 https://doi.org/10.1021/Es203658f	journal	February 2012
Formation of Mercury Sulfide from Hg(II)–Thiolate Complexes in Natural Organic Matter Manceau, Alain; Lemouchi, Cyprien; Enescu, Mironel Environmental Science & Technology, Vol. 49, Issue 16 https://doi.org/10.1021/acs.est.5b02522	journal	July 2015
Periphyton Biofilms Influence Net Methylmercury Production in an Industrially Contaminated System Olsen, Todd A.; Brandt, Craig C.; Brooks, Scott C. Environmental Science & Technology, Vol. 50, Issue 20 https://doi.org/10.1021/acs.est.6b01538	journal	September 2016
Thermodynamic Modeling of the Solubility and Chemical Speciation of Mercury and Methylmercury Driven by Organic Thiols and Micromolar Sulfide Concentrations in Boreal Wetland Soils Liem-Nguyen, Van; Skyllberg, Ulf; Björn, Erik Environmental Science & Technology, Vol. 51, Issue 7 https://doi.org/10.1021/acs.est.6b04622	journal	March 2017
Total Mercury Released to the Environment by Human Activities Streets, David G.; Horowitz, Hannah M.; Jacob, Daniel J. Environmental Science & Technology, Vol. 51, Issue 11 https://doi.org/10.1021/acs.est.7b00451	journal	May 2017
Effects of Sulfide Concentration and Dissolved Organic Matter Characteristics on the Structure of Nanocolloidal Metacinnabar Poulin, Brett A.; Gerbig, Chase A.; Kim, Christopher S. Environmental Science & Technology, Vol. 51, Issue 22 https://doi.org/10.1021/acs.est.7b02687	journal	October 2017
Sulfurization of Dissolved Organic Matter Increases Hg–Sulfide–Dissolved Organic Matter Bioavailability to a Hg-Methylating Bacterium Graham, Andrew M.; Cameron-Burr, Keaton T.; Hajic, Hayley A. Environmental Science & Technology, Vol. 51, Issue 16 https://doi.org/10.1021/acs.est.7b02781	journal	July 2017
Thermodynamics of Hg(II) Bonding to Thiol Groups in Suwannee River Natural Organic Matter Resolved by Competitive Ligand Exchange, Hg L _III -Edge EXAFS and ¹ H NMR Spectroscopy Song, Yu; Jiang, Tao; Liem-Nguyen, Van Environmental Science & Technology, Vol. 52, Issue 15 https://doi.org/10.1021/acs.est.8b00919	journal	July 2018
Mercury Sorption and Desorption on Organo-Mineral Particulates as a Source for Microbial Methylation Zhang, Lijie; Wu, Shan; Zhao, Linduo Environmental Science & Technology, Vol. 53, Issue 5 https://doi.org/10.1021/acs.est.8b06020	journal	January 2019
Binding of Mercury(II) to Dissolved Organic Matter: The Role of the Mercury-to-DOM Concentration Ratio Haitzer, Markus; Aiken, George R.; Ryan, Joseph N. Environmental Science & Technology, Vol. 36, Issue 16 https://doi.org/10.1021/es025699i	journal	August 2002
Formation of Nanocolloidal Metacinnabar in Mercury-DOM-Sulfide Systems Gerbig, Chase A.; Kim, Christopher S.; Stegemeier, John P. Environmental Science & Technology, Vol. 45, Issue 21 https://doi.org/10.1021/es201837h	journal	November 2011
Methylation of Mercury by Bacteria Exposed to Dissolved, Nanoparticulate, and Microparticulate Mercuric Sulfides Zhang, Tong; Kim, Bojeong; Levard, Clément Environmental Science & Technology, Vol. 46, Issue 13 https://doi.org/10.1021/es203181m	journal	January 2012
Refining Thermodynamic Constants for Mercury(II)-Sulfides in Equilibrium with Metacinnabar at Sub-Micromolar Aqueous Sulfide Concentrations Drott, A.; Björn, E.; Bouchet, S. Environmental Science & Technology, Vol. 47, Issue 9 https://doi.org/10.1021/es304824n	journal	April 2013
Dissolved Organic Matter Kinetically Controls Mercury Bioavailability to Bacteria Chiasson-Gould, Sophie A.; Blais, Jules M.; Poulain, Alexandre J. Environmental Science & Technology, Vol. 48, Issue 6 https://doi.org/10.1021/es4038484	journal	February 2014
Identification of Multiple Mercury Sources to Stream Sediments near Oak Ridge, TN, USA Donovan, Patrick M.; Blum, Joel D.; Demers, Jason D. Environmental Science & Technology, Vol. 48, Issue 7 https://doi.org/10.1021/es4046549	journal	March 2014
Tracing Mercury Contamination from the Idrija Mining Region (Slovenia) to the Gulf of Trieste Using Hg Isotope Ratio Measurements Foucher, Delphine; Hintelmann, Holger Environmental Science & Technology, Vol. 43, Issue 1 https://doi.org/10.1021/es801772b	journal	January 2009
Mercury Cycling in Stream Ecosystems. 1. Water Column Chemistry and Transport Brigham, Mark E.; Wentz, Dennis A.; Aiken, George R. Environmental Science & Technology, Vol. 43, Issue 8 https://doi.org/10.1021/es802694n	journal	April 2009
Formation of Mercuric Sulfide in Soil Barnett, Mark O.; Harris, Lawerence A.; Turner, Ralph R. Environmental Science & Technology, Vol. 31, Issue 11 https://doi.org/10.1021/es960389j	journal	November 1997
Enhanced Dissolution of Cinnabar (Mercuric Sulfide) by Dissolved Organic Matter Isolated from the Florida Everglades Ravichandran, Mahalingam; Aiken, George R.; Reddy, Michael M. Environmental Science & Technology, Vol. 32, Issue 21 https://doi.org/10.1021/es9804058	journal	November 1998
Nuclear magnetic resonance studies of the solution chemistry of metal complexes. 25. Hg(thiol)3 complexes and HG(II)-thiol ligand exchange kinetics Cheesman, Bruce V.; Arnold, Alan P.; Rabenstein, Dallas L. Journal of the American Chemical Society, Vol. 110, Issue 19 https://doi.org/10.1021/ja00227a014	journal	September 1988
Microbial methylation potential of mercury sulfide particles dictated by surface structure Tian, Li; Guan, Wenyu; Ji, Yunyun Nature Geoscience, Vol. 14, Issue 6 https://doi.org/10.1038/s41561-021-00735-y	journal	April 2021
Nucleation of mercury sulfide by dealkylation Enescu, Mironel; Nagy, Kathryn L.; Manceau, Alain Scientific Reports, Vol. 6, Issue 1 https://doi.org/10.1038/srep39359	journal	December 2016
Hg isotopes reveal in-stream processing and legacy inputs in East Fork Poplar Creek, Oak Ridge, Tennessee, USA Demers, Jason D.; Blum, Joel D.; Brooks, Scott C. Environmental Science: Processes & Impacts, Vol. 20, Issue 4 https://doi.org/10.1039/c7em00538e	journal	January 2018
Crystal lattice defects in nanocrystalline metacinnabar in contaminated streambank soils suggest a role for biogenic sulfides in the formation of mercury sulfide phases Koenigsmark, Faye; Chiu, Michelle; Rivera, Nelson Environmental Science: Processes & Impacts, Vol. 25, Issue 3 https://doi.org/10.1039/d1em00549a	journal	January 2023
Thermodynamic stability of mercury(II) complexes formed with environmentally relevant low-molecular-mass thiols studied by competing ligand exchange and density functional theory Liem-Nguyen, Van; Skyllberg, Ulf; Nam, Kwangho Environmental Chemistry, Vol. 14, Issue 4 https://doi.org/10.1071/En17062	journal	January 2017
Suwannee River Natural Organic Matter: Isolation of the 2R101N Reference Sample by Reverse Osmosis Green, Nelson W.; McInnis, Daniel; Hertkorn, Norbert Environmental Engineering Science, Vol. 32, Issue 1 https://doi.org/10.1089/ees.2014.0284	journal	January 2015
The Chemical Cycle and Bioaccumulation of Mercury Morel, François M. M.; Kraepiel, Anne M. L.; Amyot, Marc Annual Review of Ecology and Systematics, Vol. 29, Issue 1 https://doi.org/10.1146/annurev.ecolsys.29.1.543	journal	November 1998
Evaluation of Lower East Fork Poplar Creek Mercury Sources Watson, David B.; Brooks, Scott C.; Mathews, Teresa J. https://doi.org/10.2172/1257903	report	June 2016

Similar Records

Evaluation of Lower East Fork Poplar Creek Mercury Sources

Technical Report · Wed Jun 01 04:00:00 UTC 2016 · OSTI ID:1257903

Watson, David B.; Brooks, Scott C.; Mathews, Teresa J.; +5 more

Interaction of Soil Microbes with Organoclays and their Impact on the Immobilization of Hg under Aerobic Conditions

Journal Article · Wed Apr 14 00:00:00 UTC 2021 · Water, Air and Soil Pollution · OSTI ID:1788241

Egbo, Timothy E.; Johs, Alexander; Sahu, Rajnish; +3 more

History of mercury use and environmental contamination at the Oak Ridge Y-12 Plant

Journal Article · Fri Jan 01 04:00:00 UTC 2010 · Environmental Pollution · OSTI ID:1037053

Brooks, Scott C; Southworth, George R

Related Subjects

54 ENVIRONMENTAL SCIENCES
freshwater
mercury
natural organic matter
soil

Title: Mobilization of mercury from contaminated creekbank soils

Citation Formats

References (46)

Similar Records

Related Subjects