Advertisement

Shooting range contamination: mobility and transport of lead (Pb), copper (Cu) and antimony (Sb) in contaminated peatland

  • Gudny Okkenhaug
  • Andreas Botnen Smebye
  • Thomas Pabst
  • Carl Einar Amundsen
  • Hilmar Sævarsson
  • Gijs D. Breedveld
Sustainable Risk Management of Contaminated Land and Sediment - NORDROCS 2016

Abstract

Purpose

Small arm shooting ranges located in peatland areas are gathering increased attention due to severe metal and antimony (Sb) contamination and challenging conditions for remediation. The goal of the present study was to gain further understanding of the distribution, binding and transport of lead (Pb), copper (Cu) and Sb in peatland contaminated by small arm shooting range activities.

Materials and methods

A field experiment was carried out at a recently closed shooting range facility in Norway, including (i) peat soil sampling for various selective extractions (water, chemical extractions, extractions by diffusive gradients in thin films, DGT), (ii) establishing groundwater wells for groundwater sampling and monitoring of groundwater level and (iii) sampling of water and sediments in surface water. The results from groundwater monitoring were used to carry out hydrogeological numerical simulations using Seep/W and CTran/W. These models were used to evaluate the residence time of the contaminants in the peatland.

Results and discussion

Increased metal concentrations were observed in the top layer of the peatland, indicating low vertical transport. Groundwater revealed high concentrations of Pb (22 ± 5 μg/L), Cu (16 ± 6 μg/L) and Sb (11 ± 2 μg/L), the dominating contaminant source to the downstream surface water. Hydrogeological modelling indicated that transport mainly happened in the upper peat layer, as a result of a higher hydraulic conductivity close to the surface and a high groundwater table. Pb (6.9 ± 0.1 μg/L), Cu (24.0 ± 0.0 μg/L) and Sb (7.4 ± 0.1 μg/L) concentrations in the stream samples confirmed the spreading of contaminants at levels toxic to aquatic organisms. Pb and Cu were most likely associated with dissolved organic carbon (DOC), whereas Sb showed no correlation with DOC.

Conclusions

The elements contaminating the peatland may leak to the nearby water course over a long-term period. Copper showed the highest concentration in the stream water despite considerably higher levels of Pb in the peat soil. Strong complexation of Cu to dissolved organic matter might explain this observation. Only a little fraction of the contaminants is transported in a particulate form, and therefore are increased sedimentation measures not considered as viable remediation option.

Keywords

Antimony Copper Lead Mobility Peatland Shooting range soil 

Notes

Acknowledgements

Financial support was provided by the Norwegian Defence Estate Agency and NGI. The authors thank Karl Andreas Jensen, Irene Eriksen Dahl and Solfid Lohne for all the valuable help with the laboratory work at NMBU. Jan Birger Voldmo is thanked for all field assistance in connection with field work at Terningmoen. We would also like to thank Professor Jan Mulder at the University of Life Sciences in Ås and Professor Rolf David Vogt at the University of Oslo for fruitful and insightful discussions.

Supplementary material

11368_2017_1739_MOESM1_ESM.docx (196 kb)
ESM 1 (DOCX 195 kb).

References

  1. Ackermann S, Giere R, Newville M, Majzlan J (2009) Antimony sinks in the weathering crust of bullets from Swiss shooting ranges. Sci Total Environ 407:1669–1682CrossRefGoogle Scholar
  2. Bartles JM, Bigham JM (1996) Methods of soil analysis part 3. Chemical methods. Soil Science Society of America, Inc., WisconsinGoogle Scholar
  3. Beckwith CW, Baird AJ, Heathwaite AL (2003) Anisotropy and depth-related heterogeneity of hydraulic conductivity in a bog peat. I: laboratory measurements. Hydrol Process 17:89–101CrossRefGoogle Scholar
  4. Bolstad M (2015) Kunnskapsstatus og kunnskapsbehov knytt til grunnforureining ved skytebaner. Utgreiing om problemomfang og kunnskapsgrunnlag (in Norwegian). Forsvarsbygg Futura rapport 2013/508, OsloGoogle Scholar
  5. Broder T, Biester H (2015) Hydrologic controls on DOC, As and Pb export from a polluted peatland—the importance of heavy rain events, antecedent moisture conditions and hydrological connectivity. Biogeosciences 12:4651–4664CrossRefGoogle Scholar
  6. Cao XD, Ma LQ, Chen M, Hardison DW, Harris WG (2003) Lead transformation and distribution in the soils of shooting ranges in Florida, USA. Sci Total Environ 307:179–189CrossRefGoogle Scholar
  7. Chao TT, Zhou L (1983) Extraction techniques for selective dissolution of amorphous iron-oxides from soils and sediments. Soil Sci Soc Am J 47:225–232CrossRefGoogle Scholar
  8. Chason DB, Siegel DI (1986) Hydraulic conductivity and related physical properties of peat, Lost River peatland, northern Minnesota. Soil Sci 142:91–99CrossRefGoogle Scholar
  9. Clausen JL, Bostick B, Korte N (2011) Migration of lead in surface water, pore water, and groundwater with a focus on firing ranges. Crit Rev Environ Sci Technol 41:1397–1448CrossRefGoogle Scholar
  10. Conesa HM, Wieser M, Gasser M, Hockmann K, Evangelou MWH, Studer B, Schulin R (2010) Effects of three amendments on extractability and fractionation of Pb, Cu, Ni and Sb in two shooting range soils. J Hazard Mater 181:845–850CrossRefGoogle Scholar
  11. Davison W, Zhang H (1994) In-situ speciation measurements of trace components in natural waters using thin-film gels. Nature 367:546–548CrossRefGoogle Scholar
  12. DGT Research (2017): DGT—for measurements in water, soils and sediments, www.dgtresearch.com
  13. Egner H, Riehm H, Domingo WR (1960) Untersuchungen über die chemische Boden-Analyse als Grundlage für die Beurteilung des Nährstoffzustandes der Boden. Annals of the Royal Swedish Agricultural College 26:199–215Google Scholar
  14. Ferlatte M, Quillet A, Larocque M, Cloutier V, Pellerin S, Paniconi C (2015) Aquifer-peatland connectivity in southern Quebec (Canada). Hydrol Process 29:2600–2612CrossRefGoogle Scholar
  15. Filella M, Williams PA, Belzile N (2009) Antimony in the environment: knowns and unknowns. Environ Chem 6:95–105CrossRefGoogle Scholar
  16. Fraser CJD, Roulet NT, Lafleur M (2001) Groundwater flow patterns in a large peatland. J Hydrol 246:142–154CrossRefGoogle Scholar
  17. Fritzsche A, Schroder C, Wieczorek AK, Handel M, Ritschel T, Totsche KU (2015) Structure and composition of Fe-OM co-precipitates that form in soil-derived solutions. Geochim Cosmochim Acta 169:167–183CrossRefGoogle Scholar
  18. Gleyzes C, Tellier S, Astruc M (2002) Fractionation studies of trace elements in contaminated soils and sediments: a review of sequential extraction procedures. Trac-Trends Anal Chem 21:451–467CrossRefGoogle Scholar
  19. Grybos M, Davranche M, Gruau G, Petitjean P, Pedrot M (2009) Increasing pH drives organic matter solubilization from wetland soils under reducing conditions. Geoderma 154:13–19CrossRefGoogle Scholar
  20. Gustafsson JP (2012) Visual MINTEQ ver. 3.0. KTH, StockholmGoogle Scholar
  21. Håkanson L (1976) A bottom sediment trap for recent sedimentary deposits. Limnol Oceanogr 21:170–174CrossRefGoogle Scholar
  22. Heier LS, Lien IB, Stromseng AE, Ljones M, Rosseland BO, Tollefsen KE, Salbu B (2009) Speciation of lead, copper, zinc and antimony in water draining a shooting range-time dependant metal accumulation and biomarker responses in brown trout (Salmo trutta L.) Sci Total Environ 407:4047–4055CrossRefGoogle Scholar
  23. Heier LS, Meland S, Ljones M, Salbu B, Stromseng AE (2010) Short-term temporal variations in speciation of Pb, Cu, Zn and Sb in a shooting range runoff stream. Sci Total Environ 408:2409–2417CrossRefGoogle Scholar
  24. Heikkilä R, Lindholm T, Tahvanainen T (2006) Mires of Finland—daughters of the Baltic Sea, The Finnish EnvironmentGoogle Scholar
  25. Hobbs NB (1986) Mire morphology and the properties and behavior of some British and foreign peats. Q J Eng Geol 19:7–80CrossRefGoogle Scholar
  26. Hockmann K, Lenz M, Tandy S, Nachtegaal M, Janousch M, Schulin R (2014) Release of antimony from contaminated soil induced by redox changes. J Hazard Mater 275:215–221CrossRefGoogle Scholar
  27. Ingram HAP (1983) Hydrology. In: Gore AJP (ed) Ecosystems of the world 4A mires: swamp, bog, fen and moor. Elsevier, Amstemdam, pp 67–158Google Scholar
  28. Johnson CA, Moench H, Wersin P, Kugler P, Wenger C (2005) Solubility of antimony and other elements in samples taken from shooting ranges. J Environ Qual 34:248–254Google Scholar
  29. Jordan RN, Yonge DR, Hathhorn WE (1997) Enhanced mobility of Pb in the presence of dissolved natural organic matter. J Contam Hydrol 29:59–80CrossRefGoogle Scholar
  30. Kellner E (2003) Wetlands-different types, their properties and functions. SKB TR-04-08, Svensk Kärnbränslehantering ABGoogle Scholar
  31. Klima og miljødepartementet (2004) Forskrift om begrensning av forurensning (Pollution Regulation), FOR 2004-06-01 nr 931. Ministry of Climate and Environment, OsloGoogle Scholar
  32. Logan EM, Pulford ID, Cook GT, MacKenzie AB (1997) Complexation of Cu2+ and Pb2+ by peat and humic acid. Eur J Soil Sci 48:685–696CrossRefGoogle Scholar
  33. Ma LQ, Hardison DW, Harris WG, Cao XD, Zhou QX (2007) Effects of soil property and soil amendment on weathering of abraded metallic Pb in shooting ranges. Water Air Soil Pollut 178:297–307CrossRefGoogle Scholar
  34. Mariussen E, Ljones M, Stromseng AE (2012) Use of sorbents for purification of lead, copper and antimony in runoff water from small arms shooting ranges. J Hazard Mater 243:95–104CrossRefGoogle Scholar
  35. Mariussen E, Vaa Johnsen I, Stromseng AE (2017) Distribution and mobility of lead (Pb), copper (Cu), zinc (Zn), and antimony (Sb) from ammunition residues on shooting ranges for small arms located on mires. Environ Sci Pollut Res 24:10182–10196CrossRefGoogle Scholar
  36. Miljødirektoratet (2016) Grenseverdier for klassifisering av vann, sediment og biota (in Norwegian). Report M-608/2016. Norwegian Environment Agency, OsloGoogle Scholar
  37. Milne CJ, Kinniburgh DG, Van Riemsdijk WH, Tipping E (2003) Generic NICA-Donnan model parameters for metal-ion binding by humic substances. Environ Sci Technol 37:958–971CrossRefGoogle Scholar
  38. Mohr CW, Vogt RD, Royset O, Andersen T, Parekh NA (2015) An in-depth assessment into simultaneous monitoring of dissolved reactive phosphorus (DRP) and low-molecular-weight organic phosphorus (LMWOP) in aquatic environments using diffusive gradients in thin films (DGT). Environ Sci-Process Impacts 17:711–727CrossRefGoogle Scholar
  39. Njåstad O, Steinnes E, Bølviken B, Økdegård M (1994) Landsomfattende kartlegging av elementsammensetning i naturlig jord: Resultater fra prøver innsamlet i 1977 og 1985 oppnådd ved ICP emisjonsspektrometri. Norges Geologiske Undersøkelse rapport nr. 94.027 (in Norwegian)Google Scholar
  40. Okkenhaug G, Amstatter K, Bue HL, Cornelissen G, Breedveld GD, Henriksen T, Mulder J (2013) Antimony (Sb) contaminated shooting range soil: Sb mobility and immobilization by soil amendments. Environ Sci Technol 47:6431–6439Google Scholar
  41. Okkenhaug G, Gebhardt KAG, Amstaetter K, Bue HL, Herzel H, Mariussen E, Almas AR, Cornelissen G, Breedveld GD, Rasmussen G, Mulder J (2016) Antimony (Sb) and lead (Pb) in contaminated shooting range soils: Sb and Pb mobility and immobilization by iron based sorbents, a field study. J Hazard Mater 307:336–343CrossRefGoogle Scholar
  42. Ottesen RT, Alexander J, Joranger T, Anderson M (2007) Proposed soil guidelines. NGU report 2007-019. Norges Geologiske Undersøkelser, TrondheimGoogle Scholar
  43. Päivänen J (1973) Hydraulic conductivity and water retention in peat soils. Acta For Fenn 129:1–70Google Scholar
  44. Palmer K, Ronkanen AK, Klove B (2015) Efficient removal of arsenic, antimony and nickel from mine wastewaters in Northern treatment peatlands and potential risks in their long-term use. Ecol Eng 75:350–364CrossRefGoogle Scholar
  45. Paquin PR et al (2002) The biotic ligand model: a historical overview. Comp Biochem Physiol C-Toxicol Pharmacol 133:3–35CrossRefGoogle Scholar
  46. van Reeuwijk LP (1995) Procedures for soil analysis. 5th edition. Chap. 12–2. Acid oxalate extraction. Technical paper 9. International Soil Reference and Information Centre, FAO, WageningenGoogle Scholar
  47. Reimann C, Matschullat J, Birke M, Salminen R (2010) Antimony in the environment: lessons from geochemical mapping. Appl Geochem 25:175–198CrossRefGoogle Scholar
  48. Rothwell JJ, Evans MG, Daniels SM, Allott TEH (2007) Baseflow and stormflow metal concentrations in streams draining contaminated peat moorlands in the Peak District National Park (UK). J Hydrol 341:90–104CrossRefGoogle Scholar
  49. Rydin H, Jeglum JK (2013) The biology of peatlands. Oxford University Press, LondonCrossRefGoogle Scholar
  50. Saar RA, Weber JH (1980) Lead (II) complexation by fulvic acid—how it differs from fulvic acid complexation of copper(II) and cadmium(II). Geochim Cosmochim Acta 44:1381–1384CrossRefGoogle Scholar
  51. Scheinost AC, Rossberg A, Vantelon D, Xifra I, Kretzschmar R, Leuz AK, Funke H, Johnson CA (2006) Quantitative antimony speciation in shooting-range soils by EXAFS spectroscopy. Geochim Cosmochim Acta 70:3299–3312CrossRefGoogle Scholar
  52. Seo DC, Yu K, DeLaune RD (2008) Comparison of monometal and multimetal adsorption in Mississippi River alluvial wetland sediment: batch and column experiments. Chemosphere 73:1757–1764CrossRefGoogle Scholar
  53. Shotyk W, Krachler M, Chen B (2004) Antimony in recent, ombrotrophic peat from Switzerland and Scotland: comparison with naturlal background values (5,320 to 8,020 14C yr BP) and implications for the global atmospheric Sb cycle. Glob Biogeochem Cycles 18:GB1016CrossRefGoogle Scholar
  54. Silamikele I, Nikodemus O, Kalinina L, Kuske E, Rodinovs V, Purmalis O, Klavins M (2011) Major and trace element distribution in the peat from omrotropic bogs in Latvia. J Environ Sci Health Part A 46:805–812CrossRefGoogle Scholar
  55. Sorvari J (2007) Environmental risks at Finnish shooting ranges—a case study. Hum Ecol Risk Assess 13:1111–1146CrossRefGoogle Scholar
  56. Sorvari J, Antikainen R, Pyy O (2006) Environmental contamination at Finnish shooting ranges—the scope of the problem and management options. Sci Total Environ 366:21–31CrossRefGoogle Scholar
  57. Steely S, Amarasiriwardena D, Xing BS (2007) An investigation of inorganic antimony species and antimony associated with soil humic acid molar mass fractions in contaminated soils. Environ Pollut 148:590–598CrossRefGoogle Scholar
  58. Stromseng AE, Ljones M, Bakka L, Mariussen E (2009) Episodic discharge of lead, copper and antimony from a Norwegian small arm shooting range. J Environ Monit 11:1259–1267CrossRefGoogle Scholar
  59. Strømseng AE, Ljønes M, Mariussen E (2014) Implementation of various initiatives at former shooting ranges established in peatlands polluted by heavy metals. Report: 2014/00604. Norwegian Defence Research Establishment, KjellerGoogle Scholar
  60. Tella M, Pokrovski GS (2012) Stability and structure of pentavalent antimony complexes with aqueous organic ligands. Chem Geol 292:57–68CrossRefGoogle Scholar
  61. Tipping E, Rieuwerts J, Pan G, Ashmore MR, Lofts S, Hill MTR, Farago ME, Thornton I (2003) The solid-solution partitioning of heavy metals (Cu, Zn, Cd, Pb) in upland soils of England and Wales. Environ Pollut 125:213–225CrossRefGoogle Scholar
  62. Xifra Olivé I (2006) Mobility of lead and antimony in shooting range soils. Doctoral thesis. Swiss Federal Institute of Technology, ZurichGoogle Scholar

Copyright information

© Springer-Verlag Berlin Heidelberg 2017

Authors and Affiliations

  1. 1.Department of Environmental EngineeringNorwegian Geotechnical Institute (NGI)OsloNorway
  2. 2.Faculty of Environmental Sciences and Natural Resource ManagementNorwegian University of Life Sciences (NMBU)ÅsNorway
  3. 3.Department of Civil, Geological and Mining EngineeringPolytechnique MontrealMontrealCanada
  4. 4.Norwegian Defence Estates AgencyOsloNorway
  5. 5.Lindum ASDrammenNorway
  6. 6.Department of GeosciencesUniversity of Oslo (UiO)OsloNorway

Personalised recommendations