Speciation and partitioning of uranium in waterbodies near Ranger Uranium Mine
Scott A. McMaster A C , Barry N. Noller B , Chris L. Humphrey A , Melanie A. Trenfield A and Andrew J. Harford AA Environmental Research Institute of the Supervising Scientist (ERISS), GPO Box 461, Darwin, NT 0801, Australia.
B Centre for Mine Land Rehabilitation Sustainable Minerals Institute, The University of Queensland, Brisbane, Qld 4072, Australia.
C Corresponding author. Email: scott.mcmaster@awe.gov.au
Environmental Chemistry 18(1) 12-19 https://doi.org/10.1071/EN20096
Submitted: 30 June 2020 Accepted: 16 September 2020 Published: 16 October 2020
Environmental context. As a part of the rehabilitation of Ranger Uranium Mine, Northern Australia, closure criteria for water concentrations of uranium and other contaminants in local waterbodies have been developed. Increased concentrations of uranium in the water column can result in an accumulation of uranium in the sediment and be hazardous to benthic organisms. A uranium partitioning relationship was derived to predict sediment uranium concentrations from water column concentrations.
Abstract. After almost four decades of mineral processing, the Ranger Uranium Mine (RUM) is set to cease operations in 2021. Beyond this period, rehabilitation of the Ranger Project Area (RPA) will continue into 2026. As part of the rehabilitation of RUM, water quality guideline values (WQGVs) for U and other metals in local waterbodies have been developed to protect aquatic organisms from the effects of metal toxicity. However, benthic organisms will also be exposed to U as it partitions from the water column to the sediments. This important component of the ecosystem may then be exposed to increased U concentrations through ingestion and adsorption of U from sediments. As increased concentrations of U in the water column can result in an accumulation of U in sediment, a U partitioning relationship was derived to enable prediction of sediment U concentrations when water column concentrations were at the WQGV. In this work, the effect of U counter ions and dissolved organic carbon on uranium speciation was modelled and demonstrated a high affinity for the formation of uranyl-organic complexes. Uranium partitioning was studied using experimental U-spiked sediment data as well as water/sediment data collected from multiple sites on and adjacent to the RPA. Using a Freundlich isotherm, and a water-column U concentration of 2.8 µg L−1 (representing the WQGV), the acid-extractable U in sediment was calculated to be 48 mg kg−1, i.e. lower than the interim sediment quality guideline value (SQGV) of 94 mg kg−1. This offers assurance that a WQGV implementation of 2.8 µg L−1 U will not lead to a level of U accumulation in sediment that will impact benthic communities.
References
Bone SE, Dynes JJ, Cliff J, Bargar JR (2017). Uranium(IV) adsorption by natural organic matter in anoxic sediments. Proceedings of the National Academy of Sciences of the United States of America 114, 711–716.| Uranium(IV) adsorption by natural organic matter in anoxic sedimentsCrossref | GoogleScholarGoogle Scholar | 28069941PubMed |
Crawford SE, Lofts S, Liber K (2017). The role of sediment properties and solution pH in the adsorption of uranium(VI) to freshwater sediments. Environmental Pollution 220, 873–881.
| The role of sediment properties and solution pH in the adsorption of uranium(VI) to freshwater sedimentsCrossref | GoogleScholarGoogle Scholar | 27825841PubMed |
Cumberland SA, Douglas G, Grice K, Moreau JW (2016). Uranium mobility in organic matter-rich sediments: A review of geological and geochemical processes. Earth-Science Reviews 159, 160–185.
| Uranium mobility in organic matter-rich sediments: A review of geological and geochemical processesCrossref | GoogleScholarGoogle Scholar |
Cumberland SA, Etschmann B, Brugger J, Douglas G, Evans K, Fisher L, Kappen P, Moreau JW (2018). Characterization of uranium redox state in organic-rich Eocene sediments. Chemosphere 194, 602–613.
| Characterization of uranium redox state in organic-rich Eocene sedimentsCrossref | GoogleScholarGoogle Scholar | 29241135PubMed |
Dong W, Tokunaga TK, Davis JA, Wan J (2012). Uranium(VI) adsorption and surface complexation modeling onto background sediments from the F-Area Savannah River site. Environmental Science & Technology 46, 1565–1571.
| Uranium(VI) adsorption and surface complexation modeling onto background sediments from the F-Area Savannah River siteCrossref | GoogleScholarGoogle Scholar |
Du L, Li S, Li X, Wang P, Huang Z, Tan Z, Liu C, Liao J, Liu N (2017). Effect of humic acid on uranium(VI) retention and transport through quartz columns with varying pH and anion type. Journal of Environmental Radioactivity 177, 142–150.
| Effect of humic acid on uranium(VI) retention and transport through quartz columns with varying pH and anion typeCrossref | GoogleScholarGoogle Scholar | 28667877PubMed |
Gustafsson JP (2014). Visual MINTEQ version 3.1. Available at https://vminteq.lwr.kth.se/ [verified 18 September 2020]
Harford AJ, van Dam RA, Humphrey CL, Jones DR, Simpson SL, Chariton AA, Gibb KS, Stauber JL (2012). The toxicity of uranium to sediment biota of Magela Creek backflow billabong environments. In ‘ERISS research summary 2010–2011’. (Ed. SSR 203) pp. 33–40. (Supervising Scientist: Darwin)
Harford AJ, Chariton AA, Simpson SL, Humphrey CL, Stauber JL, van Dam RA (2015). The toxicity of uranium to sediment biota of Magela Creek backflow billabong environments. In ‘ERISS research summary 2013–2014’. (Ed. SSR 209) pp. 3–26. (Supervising Scientist: Darwin)
Hart BT, McGregor RJ (1982). Water quality characteristics of eight billabongs in the Magela creek catchment. Research Report 2. Supervising Scientist for the Alligator Rivers Region, Canberra, Australia.
Hein KAA (2002). Geology of the Ranger Uranium Mine, Northern Territory, Australia: structural constraints on the timing of uranium emplacement. Ore Geology Reviews 20, 83–108.
| Geology of the Ranger Uranium Mine, Northern Territory, Australia: structural constraints on the timing of uranium emplacementCrossref | GoogleScholarGoogle Scholar |
Hull LC, Grossmanb C, Fjeld RA, Coates JT, Elzerman AW (2002). ‘Estimating uranium partition coefficients from laboratory adsorption isotherms.’ (Idaho National Engineering and Environmental Laboratory: Idaho Falls, ID)
Humphrey CL, Chandler L (2018). Use of field-effects information to inform surface water guideline values for magnesium sulfate in Magela Creek. Research Report 212. Supervising Scientist Branch, Darwin, Australia.
Lenhart JJ, Honeyman BD, Cabaniss SE, MacCarthy P (2000). Uranium(VI) complexation with citric, humic and fulvic acids. Radiochimica Acta 88, 345–353.
| Uranium(VI) complexation with citric, humic and fulvic acidsCrossref | GoogleScholarGoogle Scholar |
Lovley D, Phillips E, Gorby Y, Landa E (1991). Microbial reduction of uranium. Nature 350, 413–416.
| Microbial reduction of uraniumCrossref | GoogleScholarGoogle Scholar |
Marchenko A, Truflandier LA, Autschbach J (2017). Uranyl carbonate complexes in aqueous solution and their ligand NMR chemical shifts and 17O quadrupolar relaxation studied by ab initio molecular dynamics. Inorganic Chemistry 56, 7384–7396.
| Uranyl carbonate complexes in aqueous solution and their ligand NMR chemical shifts and 17O quadrupolar relaxation studied by ab initio molecular dynamicsCrossref | GoogleScholarGoogle Scholar | 28598146PubMed |
Markich SJ (2002). Uranium Speciation and Bioavailability in Aquatic Systems: An Overview. The Scientific World Journal 2, 707–729.
| Uranium Speciation and Bioavailability in Aquatic Systems: An OverviewCrossref | GoogleScholarGoogle Scholar | 12805996PubMed |
Mühr-Ebert EL, Wagner F, Walther C (2019). Speciation of uranium: Compilation of a thermodynamic database and its experimental evaluation using different analytical techniques. Applied Geochemistry 100, 213–222.
| Speciation of uranium: Compilation of a thermodynamic database and its experimental evaluation using different analytical techniquesCrossref | GoogleScholarGoogle Scholar |
Novotnik B, Chen W, Evans RD (2018). Uranium bearing dissolved organic matter in the porewaters of uranium contaminated lake sediments. Applied Geochemistry 91, 36–44.
| Uranium bearing dissolved organic matter in the porewaters of uranium contaminated lake sedimentsCrossref | GoogleScholarGoogle Scholar |
Overall RA, Parry DL (2004). The uptake of uranium by Eleocharis dulcis (Chinese water chestnut) in the Ranger Uranium Mine constructed wetland filter. Environmental Pollution 132, 307–320.
| The uptake of uranium by Eleocharis dulcis (Chinese water chestnut) in the Ranger Uranium Mine constructed wetland filterCrossref | GoogleScholarGoogle Scholar | 15312943PubMed |
Pownceby MI, Johnson C (2014). Geometallurgy of Australian uranium deposits. Ore Geology Reviews 56, 25–44.
| Geometallurgy of Australian uranium depositsCrossref | GoogleScholarGoogle Scholar |
Selvakumar R, Ramadoss G, Mridula PM, Rajendran K, Thavamani P, Ravi N, Megharaj M (2018). Challenges and complexities in remediation of uranium contaminated soils: A review. Journal of Environmental Radioactivity 192, 592–603.
| Challenges and complexities in remediation of uranium contaminated soils: A reviewCrossref | GoogleScholarGoogle Scholar | 29525111PubMed |
Simpson SL, Batley GE) (2016). ‘Sediment quality assessment: a practical handbook.’ (CSIRO Publishing: Melbourne)
Singh K, Shah C, Dwivedi C, Kumar M, Bajaj PN (2013). Study of uranium adsorption using amidoximated polyacrylonitrile-encapsulated macroporous beads. Journal of Applied Polymer Science 127, 410–419.
| Study of uranium adsorption using amidoximated polyacrylonitrile-encapsulated macroporous beadsCrossref | GoogleScholarGoogle Scholar |
Supervising Scientist (2008). A longitudinal study of radionuclide and metal uptake in mussels from Magela Creek and Mudginberri Billabong. Annual Report 2007–2008, Commonwealth of Australia.
Sutcliffe B, Chariton AA, Harford AJ, Hose GC, Greenfield P, Elbourne LDH, Oytam Y, Stephenson S, Midgley DJ, Paulsen IT (2017). Effects of uranium concentration on microbial community structure and functional potential. Environmental Microbiology 19, 3323–3341.
| Effects of uranium concentration on microbial community structure and functional potentialCrossref | GoogleScholarGoogle Scholar | 28631400PubMed |
Takeno N (2005). ‘Atlas of Eh-pH diagrams.’ (National Institute of Advanced Industrial Science and Technology: Tokyo)
Thompson PA, Kurias J, Mihok S (2005). Derivation and use of sediment quality guidelines for ecological risk assessment of metals and radionuclides released to the environment from uranium mining and milling activities in Canada. Environmental Monitoring and Assessment 110, 71–85.
| Derivation and use of sediment quality guidelines for ecological risk assessment of metals and radionuclides released to the environment from uranium mining and milling activities in CanadaCrossref | GoogleScholarGoogle Scholar | 16308779PubMed |
Trenfield MA, McDonald S, Kovacs K, Lesher EK, Pringle JM, Markich SJ, Ng JC, Noller B, Brown PL, van Dam RA (2011). Dissolved organic carbon reduces uranium bioavailability and toxicity. 1. Characterization of an aquatic fulvic acid and its complexation with uranium[VI]. Environmental Science & Technology 45, 3075–3081.
| Dissolved organic carbon reduces uranium bioavailability and toxicity. 1. Characterization of an aquatic fulvic acid and its complexation with uranium[VI]Crossref | GoogleScholarGoogle Scholar |
USEPA (1999). Review of geochemistry and available Kd values for cadmium, cesium, chromium, lead, plutonium, radon, strontium, thorium, tritium (3H), and uranium. In ‘Understanding variations in partitioning coefficient, Kd, values’. Vol. II. (US Environmental Protection Agency: Washington, DC)
van Dam R, Trenfield M, Markich S, Harford A, Humphrey C, Hogan A, Stauber J (2012). Reanalysis of uranium toxicity data for selected freshwater organisms and the influence of dissolved organic carbon. Environmental Toxicology and Chemistry 31, 2606–2614.
| Reanalysis of uranium toxicity data for selected freshwater organisms and the influence of dissolved organic carbonCrossref | GoogleScholarGoogle Scholar | 22893585PubMed |
van Dam RA, Hogan AC, Harford AJ (2017). Development and implementation of a site-specific water quality limit for uranium in a high conservation value ecosystem. Integrated Environmental Assessment and Management 13, 765–777.
| Development and implementation of a site-specific water quality limit for uranium in a high conservation value ecosystemCrossref | GoogleScholarGoogle Scholar | 27943587PubMed |
Yasim NSEM, Ariffin NAN, Mohammed N, Ayob S (2017). Mechanism and kinetics of uranium adsorption onto soil around coal-fired power plant. AIP Conference Proceedings 1904, 020082
| Mechanism and kinetics of uranium adsorption onto soil around coal-fired power plantCrossref | GoogleScholarGoogle Scholar |