Historical Profiles of PCB in Dated Sediment Cores Suggest Recent Lake Contamination through the 'Halo Effect'

摘要

We investigated the major sources of poly-chlorinated biphenyls (PCB) and interpreted the environmental fate processes of these persistent organic pollutants in the past and current PCB contamination of three large, urbanized, French peri-alpine lakes. Dated sediment cores were analyzed in order to reconstruct and compare the historical contamination in all three lakes. Stratigraphic changes of PCB contents and fluxes were considered as revealing the temporal dynamics of PCB deposition to the lakes and the distribution of the seven indicator congeners (further referred to as PCBi) as an indicator of the main contamination origin and pathway. Although located within a single PCB industrial production region, concentration profiles for the three lakes differed in timing, peak concentration magnitudes, and in the PCBi congeners compositions. PCBi fluxes to the sediment and the magnitude of the temporal changes were generally much lower in Lake Annecy (0.05-2 ng·cm~(-2)·yr~(-1)) as compared to Lakes Geneva (0.05-5 ng·cm~(-2)·yr~(-1)) and Bourget (5-290 ng·cm~(-2)yr~(-1)). For all three lakes, the paramount contamination occurred in the early 1970s. In Lakes Annecy and Bourget, PCB fluxes have declined and plateaued at 0.5 and 8 ng·cn~(-2)·yr~(-1), respectively, since the early 1990s. In Lake Geneva, PCB fluxes have further decreased by the end of the XXth century and are now very low. For the most contaminated Iake (Lake Bourget), the high PCBi flux (5-290 ng-cm~(-2)·yr~(-1)) and the predominance of heavy congeners for most of the time period are consistent with a huge local input to the lake. This still high rate of Lake Bourget is explained by transport of suspended solids from one of its affluents, polluted by an industrial point source. Intermediate historical levels and PCBi distribution over time for Lake Geneva suggest a mixed contamination (urban point sources and distant atmospheric transport), while atmospheric deposition to Lake Annecy explains its lowest contamination rate. The presently low contamination levels recorded in Lake Geneva correspond to atmospheric inputs, but the recent PCBi distribution of Lake Annecy, enriched in relatively heavy congeners, reveals a contamination by the neighboring Lake Bourget, following a halo effect of about 40 km radius.