Apportioning atmospheric pollution to Canadian and American sources in Kejimkujik National Park, Nova Scotia, using Pb isotopes in precipitation

Abstract

Precipitation samples were collected from July 2001 through June 2002 to determine sources of anthropogenic heavy metal pollutants to Kejimkujik National Park, Nova Scotia using Pb isotope ratios. Generally, Mean annual Pb concentrations (0.116 μg l−1) and depositional fluxes (151 μg m−2) are lower than other reported mid-Atlantic coastal regions. Pb isotope compositions may be explained by binary mixing of anthropogenic emissions from US and Canadian sources, indicating long-range atmospheric transport of pollutants from populated and industrial regions of northeastern US and southeastern Canada. The 206Pb/207Pb ratios in precipitation ranged from 1.165 to 1.201, with an annual weighted mean 206Pb/207Pb ratio of 1.181, indicating that on an annual basis, US and Canadian sources contribute 61% and 39%, respectively, of the anthropogenic Pb (and likely other similarly behaved metal pollutants) reaching Kejimkujik Park. These results differ from those estimated by using epiphytic lichens due to one or a combination of the following possibilities: (1) some of the Pb in the lichens reflects more radiogenic local bedrock sources; (2) there has been an overall increase in the proportion of Canadian inputs since the early 1990s; (3) there was an unusually higher proportion of Pb inputs from Canadian sources during the study period; or (4) possible shifts in the isotopic composition of the Canadian and US sources that may have occurred due to increased international trade in lead and a lesser dependency on national production. As well, seasonal variations in the sources were observed, with summer and fall months having a lower mean 206Pb/207Pb ratio of 1.178 (more Canadian) than the winter and spring months with 206Pb/207Pb of 1.185 (more American).