Journal of Paleolimnology

, Volume 47, Issue 1, pp 101–112 | Cite as

Application of a simple binary mixing model to the reconstruction of lead pollution sources in two Mississippi River floodplain lakes

  • Richard B. Brugam
  • Michael Ketterer
  • Laylonda Maines
  • Zhi Qing Lin
  • William A. Retzlaff
Original paper


A simple binary mixing model is used to determine the isotopic ratios of lead (Pb) pollution sources to a lake located near a smelter closed because of excessive Pb aerosols (Horseshoe Lake Madison County, Illinois, USA). As a control, we also examine a relatively unpolluted lake in a rural area of Southern Illinois (Horseshoe Lake Alexander County). Sediment cores were taken from both lakes and analyzed for Pb and Pb isotopes by ICP-MS. The mixing model shows that Madison County Horseshoe Lake had 3 different sources of Pb in its history. The first source is sediment from the Mississippi River with an intermediate 206Pb/207Pb ratio (1.223 ± 0.009) which dominates inputs in pre-settlement times. From 1750 to 1933, the source of pollution Pb has the high 206Pb/207Pb ratio (1.256 ± 0.005) characteristic of ore from the southeast Missouri Pb mines. The most recently deposited pollution Pb comes from a source with a low 206Pb/207Pb ratio (1.202 ± 0.005). This source is similar in isotopic composition to pollution Pb found by several other investigators in the Eastern US and probably represents the mixture of ores used in modern industrial processes. It is unclear from the isotopic composition whether this source at Horseshoe Lake is the local Pb smelter or vehicle exhaust. The sediment core from Horseshoe Lake, Alexander County, shows a less variable isotopic composition. The binary mixing model showed a source composition of 1.225 ± 0.003 before 1850 and 1.231 ± 0.003 after this date. The change does not indicate a pollution source, but may be a shift in the sources of natural sediment with slightly different isotopic ratios to the lake. Our results show the value of simple binary mixing models to reconstruct the isotopic composition of Pb sources to lakes.


Pb isotopes Isotope mixing Illinois Pb contamination Lakes 



We thank the Southern Illinois University Center for Urban Research and its Director, Dr. Andrew Theising, for funding this research. We also thank Dr. Daniel Engstrom of the St. Croix Watershed Research Center, Marine on St. Croix, Minnesota, for dating the Horseshoe Lake Madison County cores.


  1. Aleinikoff JN, Muhs DR, Sauer RR, Fanning CM (1999) Late Quaternary loess in northeastern Colorado: Part II—Pb isotopic evidence for the variability of loess sources. Geol Soc Amer Bull 111:1876–1883CrossRefGoogle Scholar
  2. Appleby PG, Oldfield F (1978) The calculation of lead-210 dates assuming a constant rate of supply of unsupported 210Pb to the sediment. Catena 5:1–8CrossRefGoogle Scholar
  3. Bindler R (2011) Contaminated lead environments of man: reviewing the lead isotopic evidence in sediments, peat, and soils for the temporal and spatial patterns of atmospheric lead pollution in Sweden. Environ Geochem Health 33:311–329CrossRefGoogle Scholar
  4. Bindler R, Renberg I, Anderson NJ, Appleby PG, Emteryd O, Boyle J (2001) Pb isotope rations of lake sediments in West Greenland: inferences on pollution sources. Atmos Environ 35:4675–4685CrossRefGoogle Scholar
  5. Bindler RI, Renberg I, Kaminder J (2008) Bridging the gap between ancient metal pollution and contemporary biogeochemistry. J Paleolimnol 40:755–770CrossRefGoogle Scholar
  6. Brännvall M-L, Bindler R, Emteryd O, Renberg I (2001) Four thousand years of atmospheric lead pollution in Northern Europe: a summary from Swedish lake sediments. J Paleolim 25:421–435CrossRefGoogle Scholar
  7. Brugam RB, Bala I, Martin J, Vermillion B, Retzlaff W (2003) The sedimentary record of environmental contamination in Horseshoe Lake, Madison County, Illinois Trans Ill State. Acad Sci 96:205–218Google Scholar
  8. Brugam RB, Crenshaw MC, Geise LAB (2007) Historical development of the Cypress/Tupelo swamp at Horseshoe Lake, Alexander County, Illinois, USA. Wetlands 27:305–318CrossRefGoogle Scholar
  9. Carignan J, Simonetti A, Gariépy C (2002) Dispersal of atmospheric lead in Northeastern North America as recorded by epiphytic lichens. Atmos Environ 36:3759–3766CrossRefGoogle Scholar
  10. Eades LJ, Farmer JG, MacKenzie AB, Kirika A, Bailey-Watts AE (2002) Stable lead isotopic characterization of the historical record of environmental lead contamination in dated freshwater lake sediment cores from northern and central Scotland. Sci Total Environ 292:55–67CrossRefGoogle Scholar
  11. Faure G, Mensing TM (2005) Isotopes: principles and applications, 3rd edn. John Wiley and Sons, Inc, Hoboken, p 897Google Scholar
  12. Fry B (2006) Stable Isotope Ecology. Springer Science+Business Media, LLC, p 297Google Scholar
  13. Goldhaber MB, Church SE, Doe BR, Aleinikoff JN, Brannon JC, Podosek FA, Moser EL, Taylor CD, Gent CA (1995) Lead and sulfur isotope investigation of Paleozoic sedimentary rocks from the Southern Mid-continent of the United State: implications for paleolhydrology and ore genesis of the Southeast Missouri Lead Belts. Econ Geol 90:1875–1910CrossRefGoogle Scholar
  14. Graney JR, Halliday AN, Keeler GJ, Nriagu JO, Robbins JA, Norton SA (1995) Isotopic record of lead pollution in lake sediments from the northeastern United States. Geochim et Cosmochim Acta 59:1715–1728CrossRefGoogle Scholar
  15. Heiri O, Lotter AF, Lemcke G (2001) Loss on ignition as a method for estimating organic and carbonate content in sediments: reproducibility and comparability of results. J Paleolimnol 25:101–110CrossRefGoogle Scholar
  16. Hill TE, Evans RL, and Bell JS (1981) Water quality assessment of Horseshoe Lake, SWS Contract Report 249, Illinois Institute of Natural Resources, SpringfieldGoogle Scholar
  17. Kharkar DP, Thomson J, Turekian HK, Forster WO (1976) Uranium and Thorium in decay series nuclides in plankton from the Caribbean. Limnol Oceanogr 21:296–301CrossRefGoogle Scholar
  18. Komárek M, Ettler V, Chrastný V, Mihaljevič M (2008) Lead isotopes in environmental sciences. A Rev Environ Int 34:562–577Google Scholar
  19. Kylander M, Weiss DJ, Kober B (2009) Two high resolution terrestrial records of atmospheric Pb deposition from New Brunswick, Canada, and Loch Laxford. Scotland Sci Total Environ 407:1644–1657CrossRefGoogle Scholar
  20. March DD (1967) The history of missouri, vol 1. Lewis Historical Publishing Co, New York and West Palm BeachGoogle Scholar
  21. Merilaenen JJ, Kustula V, Wittick A, Haltia-Hovi E, Saarinen T (2010) Pollution history from 256 BC to AD 2005 inferred from the accumulation of elements in a varve record of Lake Korttajaervi in Finland. J Paleolimnol 44:531–545Google Scholar
  22. Michelutti N, Simonetti A, Briner JP, Funder S, Ceaser RA, Wolfe A (2009) Temporal trends of pollution Pb and other metals in east-central Baffin Island inferred from lake sediment geochemistry. Sci Total Environ 407:5653–5662CrossRefGoogle Scholar
  23. Prapaipong P, Enssle CW, Morris JD, Schock EL, Lindvall RE (2008) Rapid transport of anthropogenic lead through soils in southeast Missouri. Appl Geochem 23:2156–2190CrossRefGoogle Scholar
  24. Rabinowitz MB, Hall GS (2002) Isotopic characterization of six major brands of white basic lead carbonate paint pigments. Bull Environ Contam Toxicol 69:617–623CrossRefGoogle Scholar
  25. Rabinowitz MB, Wetherill GW (1972) Identifying sources of lead contamination by stable isotope techniques. Environ Sci Technol 6:705–709CrossRefGoogle Scholar
  26. Renberg I, Bränvall M-L, Bindler R, Emteryd O (2002) Stable lead isotopes and lake sediments—a useful combination for the study of atmospheric lead pollution history. Sci Total Environ 292:45–54CrossRefGoogle Scholar
  27. Schoolcraft HR (1819) A view of the lead mines of Missouri (1972 Reprint Edition) Arno Press, New YorkGoogle Scholar
  28. Seyferth D (2003) The rise and fall of tetraethyllead 2. Organometallics 22:5154–5178CrossRefGoogle Scholar
  29. Shotyk W, Krachler M (2010) The evolution of atmospheric Pb in central Ontario since AD 1800 and its impacts on the soils, waters and sediments of a forested watershed, Kawagama Lake. Geochim et Cosmochim Acta 24:196–1981Google Scholar
  30. Sturges WT, Barrie LA (1987) Lead 206/207 isotope ratios in the atmosphere of North America as tracers of US and Canadian emissions. Nature 129:144–146CrossRefGoogle Scholar
  31. Theising AJ (2003) East St Louis made in USA: the rise and fall of an industrial river town. Virginia Publishing, St Louis, p 235Google Scholar
  32. Townsend AT, Snape I (2002) The use of Pb isotope ratios determined by magnetic sector ICP-MS for tracing Pb pollution in marine sediments near Casey Station, East Antarctica. J Anal At Spectrom 17:922–928CrossRefGoogle Scholar
  33. USEPA (1996) Acid digestion for sediments sludge and soils Method 3050B. US Environmental Protection Agency, Washington, DCGoogle Scholar
  34. USEPA (2003) NPL Fact Sheets for Illinois: NL Industries/Taracorp Smelter EPA ID #ILD096731. US Environmental Protection Agency, Washington, DCGoogle Scholar
  35. Vermillion B, Brugam RB, Retzlaff WA, Bala I (2005) The sedimentary record of environmental lead contamination at St Louis, Missouri (USA) area smelters. J Paleolimnol 33:189–203CrossRefGoogle Scholar
  36. Watmough SA, Dillon PJ (2007) Lead biogeochemistry in a central Ontario forested watershed. Biogeochem 84:143–159CrossRefGoogle Scholar
  37. WR Brink Co (1882) History of Madison County, Illinois with Illustrations. W R Brink & Co, Edwardsville, IL, p 603Google Scholar
  38. Weiss D, Shotyk W, Boyle EA, Kramers JD, Appleby PB, Cheburkin AK (2002) Comparative study of the temporal evolution of atmospheric lead deposition in Scotland and eastern Canada using blanket peat bogs. Sci Total Environ 292:7–18CrossRefGoogle Scholar
  39. Yang H, Linge K, Rose N (2007) The Pb pollution fingerprint at Lochnagar: The historical records and current status of Pb isotopes. Environ Pollut 145:723–729CrossRefGoogle Scholar

Copyright information

© Springer Science+Business Media B.V. 2011

Authors and Affiliations

  • Richard B. Brugam
    • 1
  • Michael Ketterer
    • 2
  • Laylonda Maines
    • 1
  • Zhi Qing Lin
    • 1
  • William A. Retzlaff
    • 1
  1. 1.Southern Illinois UniversityEdwardsvilleUSA
  2. 2.Northern Arizona UniversityFlagstaffUSA

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