Methylmercury complexes: Selection of thermodynamic properties and application to the modelling of a column experiment
Résumé
Complexation with methyl groups produces the most toxic form of mercury, especially because of its capacity to bioconcentrate in living tissues. Understanding and integrating methylation and demethylation processes is of the utmost interest in providing geochemical models relevant for environmental assessment. In a first step, we investigated methylation at equilibrium, by selecting the thermodynamic properties of different complexes that form in the chemical system Hg-SO3-S-Cl-C-H2O. The selection included temperature dependencies of the equilibrium constants when available. We also considered adsorption and desorption reactions of both methylated and non-methylated mercury onto mineral surfaces. Then we assessed the kinetics of methylation by comparing a dedicated column experiment with the results of a geochemical model, including testing different methylation and demethylation kinetic rate laws. The column system was a simple medium: silicic sand and iron hydroxides spiked with a mercury nitrate solution. The modelling of methylmercury production with two different rate laws from the literature is bracketing the experimental results. Dissolved mercury, iron and sulfate concentrations were also correctly reproduced. The internal evolution of the column was also correctly modeled, including the precipitation of mackinawite (FeS) and the evolution of dissolved iron. The results validate the conceptual model and underline the capacity of geochemical models to reproduce some processes driven by bacterial activity.
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