Shotyk W, Weiss D, Heisterkamp M, Cheburkin A K, Appleby P G, Adams F C
Geological Institute, University of Berne, Switzerland.
Environ Sci Technol. 2002 Sep 15;36(18):3893-900. doi: 10.1021/es010196i.
A peat core collected at Etang de la Gruère, an ombrotrophic bog in the Jura Mountains of Switzerland, was analyzed for organolead species (DEL, TEL, DML, and TML) using GC-MIP AES, Pb isotopes using TIMS, and total Pb using XRF and age-dated using 210Pb. The earliest occurrence of quantifiable alkyllead is found at a depth of 24 cm, which is dated at AD 1946 +/- 3; this finding is consistent with the introduction of leaded gasoline in Switzerland in 1947. The maximum concentration of alkyllead (2.89 ng/g) is found at 5 cm, which is dated at AD 1988 +/- 2. This same sample yielded 206Pb/207Pb = 1.1254, which is the least radiogenic value in the entire 2K core and comparable to the isotopic composition of Pb in leaded gasoline. The highest concentrations of DML (906 ng/g) and DEL (1906 ng/g) also were found in this sample. Total alkyllead never accounts for more than 0.02% of total Pb in any given sample. The spatial and temporal variations in organolead species is matched by the changes in the isotopic composition of Pb over the same interval. Despite this, the decline in anthropogenic Pb pre-dates the maximum in total alkyllead and minimum 206Pb/207Pb, indicating that atmospheric Pb emissions had already begun their decline prior to the introduction of unleaded gasoline. In fact the decline in anthropogenic Pb was probably in response to the introduction of legislation, first in Germany and later in the European Union, establishing a maximum allowable concentration of Pb in gasoline.