Application of sorbents in different soil types from small arms shooting ranges for immobilization of lead (Pb), copper (Cu), zinc (Zn), and antimony (Sb)

  • Espen Mariussen
  • Ida Vaa Johnsen
  • Arnljot Einride Strømseng
Soils, Sec 3 • Remediation and Management of Contaminated or Degraded Lands • Research Article
  • 45 Downloads

Abstract

Purpose

Soil contamination of ammunition residues at shooting ranges for small arms may be followed by leaching of lead (Pb), copper (Cu), zinc (Zn), and antimony (Sb). Mixing stabilizing agents into the soil may reduce the mobility of the contaminants. To avoid risk of unexpected effects of a stabilizing agent in large-scale measures, the effect of an amendment should be tested on a small scale in advance. Two different amendments, ferric oxyhydroxide powder (CFH-12 from a commercial provider) and zerovalent iron (powder or grit), were mixed into different soil types in order to test their generic effects as stabilizing agents in contaminated soil from shooting ranges. Factors that were considered for their effects were soil water pH, limestone addition, soil chemical composition, and content of organic matter.

Materials and methods

The stabilizing agents (2–4% weight basis) were mixed into four different soil types contaminated with ammunition residues. The effects of the amendments were elucidated in two column experiments, one small-scale and one larger-scale experiment. Leaching of Pb, Cu, Zn, and Sb from the soil mixed with stabilizing agents was compared with reference soil with no amendments added.

Results and discussion

Best performance was achieved on leaching of Sb irrespective of the type of iron amendment and soil type. The Sb concentrations in the soil leachates were 55–94% less than in the leachates from the reference soils. Both amendments mixed into an acidic soil reduced the Pb, Cu, and Zn concentrations in the soil leachates in the range of 79–99%. The ability of the amendment to reduce leaching of Pb, Cu, and Zn from the other soil types was highly dependent on soil pH. CFH-12 was acidic and pH had to be balanced with limestone. The general trend was that the iron amendments reduced leaching of the elements in the order Sb>>Cu > Pb ≥ Zn.

Conclusions

Iron amendment may be suitable as stabilizing agents for Pb, Cu, Zn, and Sb in soil. The soil pH appeared to be the most important factor governing the mobility of the ammunition residues in the soils. Overall, best effect was achieved with zerovalent iron, which can be purchased at low cost and appeared to have minor influence on the properties of the soils.

Keywords

Antimony Heavy metals Iron oxyhydroxide Soil amendments Soil stabilization Zerovalent iron 

Notes

Acknowledgements

Dr. Gudny Okkenhaug from NGI, Norway, kindly provided the CFH-12 Fe oxyhydroxide powder and the limestone used in the study. MSc Elisabeth Elje from FFI helped in preparing and sampling in the lysimeter-2 experiment. The authors also wish to acknowledge Dr. Gudny Okkenhaug and MSc Helga Lassen Bue from NGI for helping in preparing the columns in the lysimeter-2 experiment.

Supplementary material

11368_2017_1875_MOESM1_ESM.doc (680 kb)
ESM 1 (DOC 679 kb)

References

  1. Armbruster DA, Tillman MD, Hubbs LM (1994) Limit of detection (LOD)/limit of quantification (LOQ): comparison of the empirical and the statistical methods exemplified with GC-MS assays of abused drugs. Clin Chem 40(7 Pt 1):1233–1238Google Scholar
  2. Chambers FM, Beilman DW, Yu Z (2011) Methods for determining peat humification and for quantifying peat bulk density, organic matter and carbon content for palaeostudies of climate and peatland carbon dynamics. Mires and Peat 7, Article no 7Google Scholar
  3. Christl I, Milne CJ, Kinniburgh DG, Kretzschmar R (2001) Relating ion binding by fulvic and humic acids to chemical composition and molecular size. 2. Metal binding. Environ Sci Technol 35(12):2512–2517.  https://doi.org/10.1021/es0002520 CrossRefGoogle Scholar
  4. Christl I, Metzger A, Heidmann I, Kretzschmar R (2005) Effect of humic and fulvic acid concentrations and ionic strenght on copper and lead binding. Environ Sci Technol 39(14):5319–5326.  https://doi.org/10.1021/es050018f CrossRefGoogle Scholar
  5. Doherty SJ, Tighe MK, Wilson SC (2017) Evaluation of amendments to reduce arsenic and antimony leaching from co-contaminated soils. Chemosphere 174:208–217.  https://doi.org/10.1016/j.chemosphere.2017.01.100 CrossRefGoogle Scholar
  6. Essington ME (2004) Soil and water chemistry: an integrative approach. CRC, Boca Raton ISBN 0-8493-1258-2Google Scholar
  7. Filella M, Belzile N, Chen YW (2002) Antimony in the environment: a review focused on natural waters II. Relevant solution chemistry. Earth-Sci Rev 59(1–4):265–285.  https://doi.org/10.1016/S0012-8252(02)00089-2 CrossRefGoogle Scholar
  8. Gundersen P, Steinnes E (2003) Influence of pH and TOC concentration on Cu, Zn, Cd, and Al speciation in rivers. Water Res 37(2):307–318.  https://doi.org/10.1016/S0043-1354(02)00284-1 CrossRefGoogle Scholar
  9. Hardison DW, Ma LQ, Luongo T, Harris WG (2004) Lead contamination in shooting range soils from abrasion of lead bullets and subsequent weathering. Sci Total Environ 328(1–3):175–183.  https://doi.org/10.1016/j.scitotenv.2003.12.013 CrossRefGoogle Scholar
  10. Hjortenkrans DST, Mansson NS, Bergback BG, Haggerud AV (2009) Problems with Sb analysis of environmentally relevant samples. Environ Chem 6(2):153–159.  https://doi.org/10.1071/EN08077 CrossRefGoogle Scholar
  11. Hockmann K, Tandy S, Lenz M, Reiser R, Conesa HM, Keller M, Studer B, Schulin R (2015) Antimony retention and release from drained and waterlogged shooting range soil under field conditions. Chemosphere 34:536–543CrossRefGoogle Scholar
  12. Jenkins TE, Grant CL, Brar GS, Thorne PG, Schumacher PW, Ranney TA (1997) Sampling errors associated with collection and analysis of soil samples at TNT-contaminated sites. Field Anal Chem Tech 1:151–163CrossRefGoogle Scholar
  13. Jenkins TE, Hewitt AD, Walsh ME, Ranney TA, Ramsey CA, Grant CL, Bjella KL (2005) Representative sampling for energetic compounds at military training ranges. Environ Foren 6(1):45–55.  https://doi.org/10.1080/15275920590913912 CrossRefGoogle Scholar
  14. 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(1):248–254Google Scholar
  15. Kosmulski M (2016) Isoelectric points and points of zero charge of metal (hydr)oxides: 50 years after Parks’ review. Adv Coll Inter Sci 238:1–61CrossRefGoogle Scholar
  16. Krogstad T. (1992): Methods for soil analyses [Norwegian] Report no. 6/92, Institute for Soil Sciences, Norwegian University of Life Sciences. ISSN 0803-1304Google Scholar
  17. Kumpiene J, Ore S, Renella G, Mench M, Lagerkvist A, Maurice C (2006) Assessment of zerovalent iron for stabilization of chromium, copper, and arsenic in soil. Environ Pollut 144(1):62–69.  https://doi.org/10.1016/j.envpol.2006.01.010 CrossRefGoogle Scholar
  18. Kumpiene J, Lagerkvist A, Maurice C (2008) Stabilization of As, Cr, Cu, Pb and Zn in soil using amendments—a review. Waste Manag 28(1):215–225.  https://doi.org/10.1016/j.wasman.2006.12.012 CrossRefGoogle Scholar
  19. Leuz AK, Moench H, Johnson AC (2006) Sorption of Sb(III) and Sb(V) to goethite: influence on Sb(III) oxidation and mobilization. Environ Sci Technol 40(23):7277–7282.  https://doi.org/10.1021/es061284b CrossRefGoogle Scholar
  20. Logan EM, Pulford ID, Cook GT, MacKenzie AB (1997) Complexation of Cu2+ and Pb2+ by peat and humic acid. Europe. J Soil Sci 48(4):685–696.  https://doi.org/10.1046/j.1365-2389.1997.00123.x CrossRefGoogle Scholar
  21. Manunza B, Deiana S, Maddau V, Gessa C, Seeber R (1995) Stability-constants of metal-humate complexes—titration data analyzed by bimodal gaussian distribution. Soil Sci Soc Am J 59(6):1570–1574.  https://doi.org/10.2136/sssaj1995.03615995005900060009x CrossRefGoogle Scholar
  22. Mariussen E (2012) Analysis of antimony (Sb) in environmental samples FFI-report 2012/00347. ISBN: 978-82-464-2049-3Google Scholar
  23. Mariussen E, Ljønes M, Strømseng AE (2012) Use of sorbents for purification of lead, cupper and antimony in runoff water from a small arms shooting range. J Hazard Mater 243:95–104.  https://doi.org/10.1016/j.jhazmat.2012.10.005 CrossRefGoogle Scholar
  24. Mariussen E, Johnsen IV, Strømseng AE (2015) Selective adsorption of lead, copper and antimony in runoff water from a small arms shooting range with a combination of charcoal and iron hydroxide. J Environ Manag 150:281–287.  https://doi.org/10.1016/j.jenvman.2014.10.019 CrossRefGoogle Scholar
  25. Mariussen E, Heier LS, Teien HC, Pettersen MN, Holth TF, Salbu B, Rosseland BO (2017a) Accumulation of lead (Pb) in brown trout (Salmo trutta) from a lake downstream a former shooting range. Ecotoxicol Environ Safe 135:327–336.  https://doi.org/10.1016/j.ecoenv.2016.10.008 CrossRefGoogle Scholar
  26. Mariussen E, Johnsen IV, Strømseng A (2017b) Distribution and mobility of lead (Pb), antimony (Sb) and copper (Cu) from ammunition residues on shooting ranges for small arms located on mires. Environ Sci Pollut Res 24(11):10182–10196.  https://doi.org/10.1007/s11356-017-8647-8 CrossRefGoogle Scholar
  27. McBride MB, Blasiak JJ (1979) Zinc and copper solubility as a function of ph in an acid soil. Soil Sci Soc Am J 43(5):866–870.  https://doi.org/10.2136/sssaj1979.03615995004300050009x CrossRefGoogle Scholar
  28. Myhre O, Fjellheim K, Ringnes H, Reistad T, Longva KS, Ramos TB (2013) Development of environmental performance indicators supported by an environmental information system: application to the Norwegian defence sector. Ecol Indic 29:293–306.  https://doi.org/10.1016/j.ecolind.2013.01.005 CrossRefGoogle Scholar
  29. Nakamaru YM, Peinado FJM (2017) Effect of soil organic matter on antimony bioavailability after the remediation process. Environ Pollut 228:425–432.  https://doi.org/10.1016/j.envpol.2017.05.042 CrossRefGoogle Scholar
  30. Nash MJ, Maskall JE, Hill SJ (2000) Methodologies for determination of antimony in terrestrial environmental samples. J Environ Monit 2(2):97–109.  https://doi.org/10.1039/a907875d CrossRefGoogle Scholar
  31. 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(12):6431–6439.  https://doi.org/10.1021/es302448k CrossRefGoogle Scholar
  32. Okkenhaug G, Gebhardt KA, Amstätter K, Bue HL, Herzel H, Mariussen E, Almås ÅR, Cornelissen G, Breedveld G, Rasmussen G, Mulder M (2016) Immobilization of antimony (Sb) and lead (Pb) in shooting range soils with iron based sorbents, a field study. J Hazard Mater 307:336–343.  https://doi.org/10.1016/j.jhazmat.2016.01.005 CrossRefGoogle Scholar
  33. Okkenhaug G, Smebye AB, Pabst T, Amundsen CE, Sævarsson H, Breedveld GD (2017) Shooting range contamination: mobility and transport of lead (Pb), copper (Cu) and antimony (Sb) in contaminated peatland. J Soils Sediments.  https://doi.org/10.1007/s11368-017-1739-8
  34. Qiu P, Leygraf C (2011) Initial oxidation of brass induced by humidified air. Appl Surf Sci 258(3):1235–1241.  https://doi.org/10.1016/j.apsusc.2011.09.080 CrossRefGoogle Scholar
  35. Randich E, Duerfeldt W, McLendon W, Tobin W (2002) A metallurgical review of the interpretation of bullet lead compositional analysis. Forensic Sci Int 127(3):174–191.  https://doi.org/10.1016/S0379-0738(02)00118-4 CrossRefGoogle Scholar
  36. Sanderson P, Naidu R, Bolan N, Bowman M, Mclure S (2012) Effect of soil type on distribution and bioaccessibility of metal contaminants in shooting range soils. Sci Total Environ 438:452–462.  https://doi.org/10.1016/j.scitotenv.2012.08.014 CrossRefGoogle Scholar
  37. Santillan-Medrano J, Jurinak JJ (1975) The chemistry of lead and cadmium in soil: solid phase formation. Soil Sci Soc Am Proc 39(5):851–856.  https://doi.org/10.2136/sssaj1975.03615995003900050020x CrossRefGoogle Scholar
  38. Schwertmann U, Fechter H (1982) The point of zero charge of natural and synthetic ferrihydrites and its relation to adsorbed silicate. Clay Miner 17(4):471–476.  https://doi.org/10.1180/claymin.1982.017.4.10 CrossRefGoogle Scholar
  39. 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(1):21–31.  https://doi.org/10.1016/j.scitotenv.2005.12.019 CrossRefGoogle Scholar
  40. Strømseng AE, Ljønes M, Mariussen E (2009) Episodic discharge of lead, copper and antimony from a Norwegian small arm shooting range. J Environ Monit 11(6):1259–1267.  https://doi.org/10.1039/b823194j CrossRefGoogle Scholar
  41. Stumm W (1995) The inner-sphere surface complex. In: Huang CP, O’Melia CR, Morgan JJ (eds) Aquatic chemistry, interfacial and interspecies processes. Advances in chemistry, vol 244. ACS Publication, American Chemical Society, Washington, DCGoogle Scholar
  42. Tandy S, Meier N, Schulin R (2017) Use of soil amendments to immobilize antimony and lead in moderately contaminated shooting range soils. J Hazard Mater 324(Pt B):617–625.  https://doi.org/10.1016/j.jhazmat.2016.11.034 CrossRefGoogle Scholar
  43. Vantelon D, Lanzirotti A, Scheinost AC, Kretzschmar R (2005) Spatial distribution and speciation of lead around corroding bullets in a shooting range souil studied by micro-X-ray fluorescence and absorption spectroscopy. Environ Sci Technol 39(13):4808–4815.  https://doi.org/10.1021/es0482740 CrossRefGoogle Scholar
  44. Violante A (2013) Elucidating mechanisms of competitive sorption at the mineral/water interface. Adv Agron 118:111–176.  https://doi.org/10.1016/B978-0-12-405942-9.00003-7 CrossRefGoogle Scholar
  45. Voie Ø, Strømseng A (2000). Risk assessment of the heavy metal pollution at an outdoor shooting range. (Norwegian) FFI/rapport 2000/06166 ISBN 82-464-0468-7Google Scholar

Copyright information

© Springer-Verlag GmbH Germany, part of Springer Nature 2017

Authors and Affiliations

  1. 1.Norwegian Defence Research Establishment (FFI)KjellerNorway
  2. 2.Norwegian Institute for Air Research (NILU)KjellerNorway
  3. 3.The Norwegian Water Resources and Energy Directorate (NVE)OsloNorway

Personalised recommendations