Isotopic record of lead pollution in lake sediments from the northeastern United States

Abstract

Although it is common knowledge that Pb concentrations have increased in lake sediments in the northeastern United States over the last 150 years, the processes responsible have been the subject of debate. In this study, differences in lead isotopic compositions and concentrations in sediment from large lakes (Lake Erie, Ontario, and Michigan) and small ones (Deep Lake and Lake Andrus) are used to infer temporal changes in the source(s) of anthropogenic Pb in the Great Lakes region. A natural (background) component of Pb is present in sediment deposited prior to 1860 in Lake Erie and the other lakes as indicated from low Pb concentrations and uniform lead isotopic compositions. Changes in isotopic ratios of lake sediment reflect differing sources of anthropogenic Pb superimposed on the natural component such as regional deforestation from 1860–1890 followed by coal combustion and ore smelting through 1930. Combustion of leaded gasoline was the dominant anthropogenic Pb source to the atmosphere (and by inference to lake sediment) from 1930–1980. Temporal changes in lead isotopic compositions in lake sediment suggest that the source of the Pb used in gasoline additives gradually changed from 1930 to present. The best example is a distinct shift in lead isotopic ratios in lake sediment deposited after 1970 which corresponds to increased Pb production from the Viburnum Trend deposits in Missouri (present in all lakes except Ontario). However, the changes in lead isotopic compositions are much less variable than and do not parallel those calculated on the basis of annual United States mine production and imports. Rather, anthropogenic recycling of Pb as well as natural mixing processes during emission, transport, and deposition of Pb in lake sediment control most of the variation in lead isotope ratios. Differences in lead isotopic ratios in Lake Michigan, Erie, and Deep Lake sediment preserve regional differences in lead isotopic ratios from U.S. and Canadian sources first noted in aerosols by Sturges and Barrie (1987). More localized sources of Pb (such as point discharges) are needed to explain the results from Lake Ontario and Andrus.