One hundred fifty-year record of lead isotopes in Antarctic snow from Coats Land

A record of the concentrations of Pb and Ba and the isotopic composition of Pb has been established for a remote, low accumulation site in the Atlantic sector of Antarctica (Coats Land) by means of thermal ionization mass spectrometry. The snow samples cover the period ∼1840 to 1990. They were taken from the walls of a pit to a depth of 7.8 m and as a core to 16 m; ultraclean procedures were used. Detailed laboratory subsampling provided both long-term (secular scale) and short-term (intra-annual) Pb, Ba, and Pb isotope variations. The results show that there have been significant variations in Pb concentrations (range, 0.1 to 9.3 pg/g) and isotopic composition (range, 1.096 to 1.208 for ²⁰⁶Pb/²⁰⁷Pb ratio) since the 1840s. The data show evidence of pollution for this metal in Antarctica as early as the 1880s. Several Pb maxima were observed: the first at the beginning of the 20th century and the last in the 1970s to 1980s, with a clear decrease during recent years. Although the last maximum is clearly linked to the rise and fall in the use of leaded gasoline in the Southern Hemisphere, especially in South America, the reason for the first remains uncertain. The pattern of changing isotopic composition of Pb reveals the changing origin and character of the anthropogenic inputs to Antarctica. An interesting feature in this pattern is the relatively large contribution of unradiogenic Pb in the ∼1890s, possibly originating from Australia. Another interesting feature is the pronounced intra-annual variation in the isotopic composition of Pb, which illustrates the complexity of the changing inputs of Pb to Antarctica.