Lead sources and transfer in the coastal Mediterranean: evidence from stable lead isotopes in marine particles

Time series of settling and suspended particles have been collected by sediment traps and in situ pumps respectively, under contrasted hydrographic conditions in the Gulf of Lions and the Ligurian Sea, northwestern Mediterranean. Lead concentrations measured in sediment trap samples vary from 41±7 ppm in the Ligurian Sea to 58±10 ppm in the Gulf of Lions. These concentrations, 2–10 times lower than those measured previously in the Gulf of Lions, reflect the reduction of lead fallout from gasoline during the last decade. While atmospheric lead still originates mainly from anthropogenic emissions (automotive and industrial exhausts), stable lead isotopes demonstrate that anthropogenic and lithogenic lead are in similar proportions in the marine particles from the northwestern Mediterranean. Sequential extraction analyses performed on trap samples suggest that the isotopic variations can be explained by a three-component mixing between anthropogenic, natural soluble, and natural refractory sources. In the suspended particulate matter from the Gulf of Lions, lead concentrations range from 0.2 to 30 ng/l, with isotopic compositions comparable to those of the settling particles (206Pb/207Pb from 1.165 to 1.178). This indicates a common origin in these two types of particles, probably mainly controlled by the Rhône River discharge and by resuspension processes on the continental shelf. By contrast, lead concentrations are lower in the suspended matter samples from the Ligurian Sea (0.5 to 1.7 ng/l). In this case, the isotopic signature (1.165±0.002) is in equilibrium with the dissolved fraction, as previously found in other oligotrophic sites in the open ocean, where the suspended particles are mainly of biological origin and lead essentially authigenic in these particles.