Geochemical distributions of natural radionuclides in surface soils and sediments impacted by lead-zinc mining activity.

This study investigated the distribution features of uranium-238 (238U), radium-226 (226Ra), thorium-232 (232Th), and potassium-40 (40K) and evaluated the associated environmental radiological hazards of the topsoil and river sediments in the Jinding lead-zinc (Pb-Zn) mine catchment from Southwest China. The activity concentrations of 238U, 226Ra, 232Th, and 40K ranged from 24.0 ± 2.29-60.3 ± 5.26 Bq.kg-1, from 32.5 ± 3.95-69.8 ± 3.39 Bq.kg-1, from 15.3 ± 2.24-58.3 ± 4.92 Bq.kg-1, and from 203 ± 10.2-1140 ± 27.4 Bq.kg-1, respectively. The highest activity concentrations for all these radionuclides were primarily found in the mining areas and decreased with increasing distance from the mining sites. The radiological hazard indices, including radium equivalent activity, absorbed gamma dose rate in the air, outdoor annual effective dose equivalent, annual gonadal dose equivalent, and excess lifetime cancer, revealed that the highest values were observed in the mining area and downstream, specifically in the vicinity of the ore body. These elevated values exceeded the global mean value but remained below the threshold value, suggesting that routine protection measures for Pb-Zn miners during production activities are sufficient. The correlation analysis and cluster analysis revealed strong associations between radionuclides such as 238U, 226Ra, and 232Th, indicating a common source of these radionuclides. The activity ratios of 226Ra/238U, 226Ra/232Th, and 238U/40K varied with distance, suggesting the influence of geological processes and lithological composition on their transport and accumulation. In the mining catchment areas, the variations in these activity ratios increased indicated the impact of limestone material dilution on the levels of 232Th, 40K, and 238U in the upstream region. Moreover, the presence of sulfide minerals in the mining soils contributed to the enrichment of 226Ra and the removal of 238U caused those activity ratios decreased in the mining areas. Therefore, in the Jinding PbZn deposit, the patterns of mining activities and surface runoff processes in the catchment area favored the accumulation of 232Th and 226Ra over 40K and 238U. This study provides the first case study on the geochemical distributions of natural radionuclides in a typical Mississippi Valley-type PbZn mining area and offers fundamental information on radionuclide migration and baseline radiometric data for PbZn deposits worldwide.

Mechanism of uranium release from uranium mill tailings under long-term exposure to simulated acid rain: Geochemical evidence and environmental implication.

To date, there is not sufficient knowledge to fully understand the occurrence, transport and fate of residual uranium (U) from uranium mill tailings (UMT). Herein this study investigated different U release behaviors from natural UMT (without grinding) under four simulated acid rain (pH = 2.0-5.0) compared with controlled scenario (pH = 6.0) for 25 weeks. The results showed that the most notable U release was observed from UMTpH2.0, followed by UMTpH3.0 whereas a nonlinear relationship between pH and U release was observed from UMTpH4.0-6.0. The divergence of U release behaviors was attributed to the presence of minerals such as calcite and clinochlore. Autunite, a secondary mineral formed after leaching, might regulate U release in UMTpH3.0-6.0. Fick theory model revealed the shift of U release mechanism from surface dissolution to diffusion transport for UMTpH2.0, UMTpH3.0 and UMTpH5.0 at varied stage, whereas UMTpH4.0 and UMTpH6.0 displayed univocal dissolution and diffusion mechanism, respectively. This study highlights the necessity of performing long-term leaching tests to detect the "shift event" of leaching kinetics and to better understand the mechanism of U release influenced by mineralogy of the natural UMT under simulated acid rain conditions, which is conducive to developing UMT management strategies to minimize the risk of U release and exposure.