Isotopic evidence of pollutant lead sources in Northwestern France

Ratios of stable lead isotopes (Pb-204, Pb-206, Pb-207, Pb-208) are used to characterize both spatial and temporal variations in anthropogenic emissions of industrial lead aerosols to the atmosphere of northwestern France. Differences in isotopic compositions of aerosols collected from a rural area (Wimereux) in the Nord-Pas de Calais region along the English Channel in 1982-1983 (Pb-206/Pb-207 = 1.108 +/- 0.005) and 1994 (Pb-206/Pb-207 = 1.148 +/- 0.003) are paralleled by similar variations in urban aerosols within France during the same period (e.g., Pb-206/Pb-207 = 1.115 +/- 0.008 from 1981-1989 and 1.143 +/- 0.006 from 1992-1995). These results correlate well with recent findings in the Mediterranean basin (Alleman, 1997) where this radiogenicity increase is clearly associated with industrial sources other than leaded gasoline that has remained relatively constant during its phasing out (Pb-206/Pb-207 = 1.08-1.11). Here we used archived data, air mass trajectories and aerosol diameters combined with isotopic signatures to confirm this trend at a regional scale. Indeed, the main industrial signatures from lead smelting (Pb-206/Pb-207 = 1.133 +/- 0.001) and steel metallurgy (Pb-206/Pb-207 = 1.196 +/- 0.015) in northwestern France appear more radiogenic than that of leaded gasoline. The shift in isotopic compositions also conform with the systematic change in the mean size (diameter) of aerosols at Wimereux, which ranged from 0.30 to 0.61 mu m in 1982-1984 and from 0.70 to 0.89 mu m in 1994. (C) 1999 Elsevier Science Ltd. All rights reserved.