Minerals controlling arsenic and lead solubility in an abandoned gold mine tailings

Numerous areas have been contaminated by heavy metals and metalloids due to industrial and mining activities. Studies investigating the behavior of such contaminants in the environment have identified speciation as a key factor controlling their mobility, availability and toxicity. Here we characterize As- and Pb-bearing phases resulting from the oxidation of sulfide-rich tailings of a former gold mine (La Petite Faye, France) in order to assess the risk for water quality. Elements were first pre-concentrated by granulometric fractionation (sedimentation in deionized water) and then investigated using X-ray diffraction and electron microprobe analyses. Two main As-Pb-bearing minerals were clearly identified: scorodite (FeAsO4 x 2H2O) and beudantite PbFe3(AsO4)(SO4)(OH)6. Minor amounts of As and Pb were dissolved in deionized water during granulometric fractionation, indicating the possible presence of other soluble Pb-sulfates which could be some of the primary metastable products of sulfide oxidation. This dissolution also provides information about the fate of these phases in the case of intensive leaching of the tailings. Scorodite may not be considered as a relevant candidate for As on-site immobilization, because its solubility largely exceeds drinking water standards whatever the pH. Since beudantite solubility has not yet been determined, an estimation of its solubility product was obtained using the Gibbs free energy of formation of plumbojarosite [Pb0.5Fe3(SO4)2(OH)6]. This estimation suggests that beudantite should efficiently maintain low Pb concentration in waters. However, Pb dissolution in deionized water during the granulometric fractionation led to Pb concentrations much higher than the French and US drinking water standards (2.4 x 10(-7) mol l(-1)), which may be due to dissolution of the suspected metastable Pb-sulfates. Accurate determination of beudantite solubility is now required to improve the Pb risk assessment on such polluted sites.