Thallium diagenesis in lacustrine sediments

摘要

Dated sediment cores and porewaters from two Canadian Shield lakes, located 40 km from Quebec City (L. Tantare) and 25 km downwind from an important smelter in northwestern Quebec (L. Vose), were analyzed for thallium and other geochemical variables. Atmospheric deposition is the only source of anthropogenic Tl to these lakes. The porewater Tl concentration profiles in L. Tantare display a peak below the sediment-water interface that suggests post-depositional Tl remobilization and transport to the overlying water and deeper sediments; such a dissolved Tl peak occurs just above the sediment-water interface in L. Vose. Modeling the porewater Tl profiles with a diagenetic reaction-transport equation reveals a zone of dissolved Tl production lying above a zone of Tl consumption in L. Tantare sediments. In contrast, in L. Vose, Tl diffuses across the sediment-water interface from the anoxic hypolimnion and is fixed to the surficial sediments. The localization of the consumption zones, the shape of the dissolved Tl, sulfide and iron profiles, as well as calculations of saturation states are all consistent with the removal of Tl from porewater by co-precipitation with and/or adsorption to Fe sulfides. The concentrations of Tl removed from or added to sediments after their deposition (i.e., diagenetic Tl) amount to up to 36% of measured sediment Tl concentrations. Comparison of the reconstructed historical Tl records with those of polycyclic aromatic hydrocarbons (PAHs) and of Pb originating from coal burning or from smelting activities indicate that coal combustion is the major source of atmospheric Tl to L. Tantare and that an additional important Tl source to L. Vose is the nearby smelter. Copyright (c) 2005 Elsevier Ltd.