Abstract: A large number of radionuclides remain in uranium tailings, and U, 226Ra and 210Pb leach out with water chemistry, causing potential radioactive contamination to the surrounding environment. In this paper, uranium tailings from a uranium tailings pond in southern China were collected at different depths by means of borehole sampling, mixed and homogenised, and analysed for mineral and chemical composition, microscopic morphology, U, 226Ra and 210Pb fugacity, static leaching and dynamic leaching of U, 226Ra and 210Pb in uranium tailings at different pH conditions. The variation of U, 226Ra and 210Pb concentrations in the leachate under different pH conditions with time was obtained, and the leaching mechanism was analysed. The results showed that the uranium tailings were dominated by quartz, plagioclase and other minerals, of which SiO2 and Al2O3 accounted for 65.45% and 13.32% respectively, and U, 226Ra and 210Pb were mainly present in the residue form. The results of the static leaching experiments show that pH mainly influences the leaching of U, 226Ra and 210Pb by changing their chemical forms and the particle properties of the tailings, and that the lower the pH the more favourable the leaching. The results of dynamic leaching experiments during the experimental cycle showed that the leaching concentration and cumulative release of U, 226Ra and 210Pb in the leach solution were greater at lower pH conditions than at higher pH conditions, and the leaching of U, 226Ra and 210Pb at different pH conditions was mainly from the water-soluble and exchangeable states. The present research results are of great significance for the environmental risk management and control of radioactive contamination in existing uranium tailings ponds, and are conducive to ensuring the long-term safety, stability and sustainability of uranium mining sites.

Abstract: VNIR-SWIR (400–2500 nm) reflectance measurements were made on the surfaces of various cores, cuttings and sample splits of sedimentary rocks from the Tertiary Jackson Group, and Catahoula, Oakville and Goliad Formations. These rocks vary in composition and texture from mudstone and claystone to sandstone and are known host rocks for roll front uranium occurrences in Karnes and Live Oak Counties, Texas. Spectral reflectance profiles, 569 in total, were reduced to 125 representative spectral signatures, which were analyzed using the U.S. Geological Survey’s (USGS) Material Identification and Characterization Algorithm (MICA). MICA uses an automated continuum-removal procedure together with a least-squares linear regression to determine the fit of observed sample spectral absorption features to those of reference mineral standards in a spectral library. The reference minerals include various clay, mica, carbonate, ferric and ferrous iron minerals and their mixtures. In addition, absorption feature band-depth analysis was done to identify rock surfaces exhibiting absorption features related to uranium and zeolite minerals, which were not included in the command files used to execute MICA. Rocks from each of the four geologic units produced broadly similar spectral signatures as a result of comparable mineral compositions, but there were some notable differences. For example, Ca- and Na-montmorillonite was matched most frequently to the spectral absorption features in 2-μm (∼2000–2500 nm) wavelengths, while goethite occurred often at 1-μm (∼400–1000 nm) wavelengths. The latter is related to limonitic iron-staining in and around oxidized zones of the uranium roll front as described in previous papers. Rocks of the Jackson Group differed from those of the Catahoula, Oakville and Goliad units in that the former exhibited spectral features we interpret as being due to the presence of lignite-bearing mudstone layers. Goliad rocks exhibit spectral features related to dolomite, gypsum, anhydrite, and an unidentified green clay mineral that is possibly glauconite. Jackson Group rocks also exhibit weak but well-resolved absorption features at 964 and 1157 nm related to either or both zeolite minerals clinoptilolite and heulandite. These zeolite minerals and a few spectra exhibiting hydrous silica absorption features are indicative of alteration of volcanic glass in tuffaceous mudstone and claystone layers. A few sample spectra exhibited strong absorption features at around 1135 nm related to the uranium mineral coffinite. Both the 1135 nm coffinite and 1157 nm zeolite absorption features overlap somewhat, potentially making them difficult to distinguish without additional hyperspectral field, laboratory or remote sensing data. The results of this study were compared to mixtures of minerals described for ore, gangue and alteration minerals in deposit models for sandstone-hosted uranium, sedimentary bentonite and sedimentary zeolite. Use of these spectra can help facilitate mapping of both waste materials from the legacy mining of the above commodities, as well as future exploration and resource assessment activities.

Abstract: The approximate determination of average Ra/U disequilibria in orebodies is one of the most common causes of errors in U reserve estimations. In roll-front deposits, the disequilibria are however frequently distributed following complex geometries, which must be fully understood to prevent major U reserve overestimates and costly unproductive extractive operations. The processes responsible for disruption of the radioactive equilibria and the U and Ra carriers in such complex natural systems remain poorly constrained. In this contribution, we propose an innovative approach, mixing orebody to sub-grain scale studies to unravel the distribution of U and Ra and the processes responsible for their concentration and uncoupling. Using mineral separations, gamma spectrometry and mineral-chemical analyses, we identified the Fe-Ti clusters (altered ilmenite + pyrite/marcasite) as the microsites for coffinite precipitation and Ra concentration. To understand the influence of such clusters on the distribution of U and Ra at the deposit scale, whole-rock Ra/U disequilibria were measured and mapped at a series of ten drill holes along a profile crosscutting the studied roll-front. The main Ra/U disequilibria are encountered around the mineralization in low U content zones. They are controlled by two main processes. (1) In the oxidized zones, the immobility of 230Th with respect to the U produces patches of Ra disequilibria (carried by the altered U minerals). (2) In the immediate vicinity of the roll-front, the dissolution of the mineralization produces an Ra flux trapped by the alteration products of ilmenites, as definitely confirmed by direct SIMS measurements. Such a process is responsible for the Ra disequilibria envelope located downstream of the richest ores, also known as Ra halo. The highest Ra/U ratios correspond to oxidized upstream samples, but most other high Ra/U ratios are from reduced downstream samples close to the mineralization. Such a low to medium U content envelope with high Ra/U ratios constitutes the main cause of U reserve overestimations.

Abstract: Sandstone uranium (U) roll-front deposits of Wyoming and Colorado (USA) are important U resources, and may provide a terrestrial source for critical accessory elements, such as selenium (Se), molybdenum (Mo), and tellurium (Te). Due to their associated toxicity, MoSeTe occurrences in roll-fronts should also be carefully monitored during U leaching and ore processing. While elevated MoSe concentrations in roll-fronts are well established, very little is known about Te occurrence in such deposits. This study aims to establish MoSeTe concentrations in Wyoming and Colorado roll-fronts, and assess the significance of these deposits in an environmental and mineral exploration context. Sampled roll-front deposits, produced by oxidized groundwater transportation through a sandstone, show high MoSe content in specific redox zones, and low Te, relative to crustal means. High Se concentrations (up to 168ppm) are restricted to a narrow band of alteration at the redox front. High Mo content (up to 115ppm) is typically associated with the reduced mineralized nose and seepage zones of the roll-front, ahead of the U orebody. Elevated trace element concentrations are likely sourced from proximal granitic intrusions, tuffaceous deposits, and local pyritic mudstones. Elevated MoSe content in the sampled roll fronts may be regarded as a contaminant in U in-situ recovery and leaching processing, and may pose an environmental threat in groundwaters and soils, so extraction should be carefully monitored. The identification of peak concentrations of MoSe can also act as a pathfinder for the redox front of a roll-front, and help to isolate the U orebody, particularly in the absence of gamma signatures.

Abstract: This study combines historical records of 14C and 3H in the atmosphere and soil with renewal rate and groundwater lumped parameter models to predict the abundance of 14C and 3H in groundwater over time. 624 groundwater samples from numerous studies, over four decades (1978–2019), in South Africa, Namibia, Botswana and Mozambique were collated to compare with predicted groundwater activities of 14C and 3H within the South African Development Community (SADC) region. Spatial datasets of carbonate bearing lithology, C3/C4 vegetation, summer/winter rainfall and coastal proximity were used to apply corrections to 14C and 3H data. Corrected values of 14C and 3H were compared with the theoretical abundance of these tracers, derived from the lumped parameter models, to estimate the general mean residence times and presence of groundwater mixing between modern recharge and older groundwaters. This study found that corrected values produced varying mean residence times derived from 14C ages (∼500–28500 years) and a wide range of potentially mixed waters within each aquifer system (0–100 % of tested wells) across the study area. The largest proportions of mixed groundwater, as well as the youngest mean residence times, were found in alluvial and primary fractured rock aquifers (e.g., western coast of South Africa and southern Mozambique). The smallest proportions of mixed groundwater were predicted in deep confined clay-rich aquifers as well as layered coal bearing carbonate sequences (e.g., Orapa, Malwewe and Serowe, Botswana). Insights into the proportions of mixed groundwater and mean residence times can help assess hydrological resilience on a regional scale. Such information is pertinent in promoting socio-economic development and increased water/food security in the SADC region. By understanding the resilience of groundwater resources, robust and informed strategies for water equality and GDP growth in the SADC region can be envisioned and implemented.