An integrated approach combining soil profile, records and tree ring analysis to identify the origin of environmental contamination in a former uranium mine (Rophin, France)

Uranium mining and milling activities raise environmental concerns due to the release of radioactive and other toxic elements. Their long-term management thus requires a knowledge of past events coupled with a good understanding of the geochemical mechanisms regulating the mobility of residual radionuclides. This article presents the results on the traces of anthropic activity linked to previous uranium (U) mining activities in the vicinity of the Rophin tailings storage site (Puy de Dôme, France). Several complementary approaches were developed based on a study of the site's history and records, as well as on a radiological and chemical characterization of soil cores and a dendrochronology. Gamma survey measurements of the wetland downstream of the Rophin site revealed a level of 1050 nSv.h−1. Soil cores extracted in the wetland showed U concentrations of up to 1855 mg.kg−1, which appears to be associated with the presence of a whitish silt loam (WSL) soil layer located below an organic topsoil layer. Records, corroborated by prior aerial photographs and analyses of 137Cs and 14C activities, suggest the discharge of U mineral particles while the site was being operated. Moreover, lead isotope ratios indicate that contamination in the WSL layer can be discriminated by a larger contribution of radiogenic lead to total lead. The dendroanalysis correlate U emissions from Rophin with the site's history. Oak tree rings located downstream of the site contain uranium concentrations ten times higher than values measured on unaffected trees. Moreover, the highest U concentrations were recorded not only for the operating period, but more surprisingly for the recent site renovations as well. This integrated approach corroborates that U mineral particles were initially transported as mineral particles in Rophin's watershed and that a majority of the deposited uranium appears to have been trapped in the topsoil layer, with high organic matter content. [Display omitted] •Origin of contamination near Rophin tailings storage site: natural vs. anthropogenic•A whitish silt loam soil layer in a wetland was associated with a high U content.•Dating and records indicate that U was deposited during previous mining activities.•U mineral particles transported by turbid waters were deposited in a wetland.•Dendroanalysis shows an uptake of 238U linked to the mining activity period.