Abstract: In-situ leaching (ISL) is a chemical method for recovering useful minerals and metals directly from underground ore bodies which is also referred to as ‘solution mining’. ISL is commonly used for uranium mining, accounting for about 45% of global production. The main benefits are claimed to be a lower environmental impact in terms of visual disturbances, emissions, lower energy use, cost compared with conventional open-cut or underground mining methods, and potential utilisation of lower grade resources. However, there is a lack of reported studies on the assessment of the environmental impacts of ISL, particularly greenhouse gas (GHG) emissions using life cycle assessment (LCA) methodology. The SimaPro LCA software was used to estimate the GHG footprint of the ISL of uranium, gold and copper. The total GHG emissions were estimated to be 38.0 kg CO2-e/kg U3O8 concentrate (yellowcake), 29 t CO2-e/kg gold, and 4.78 kg CO2-e/kg Cu. The GHG footprint of ISL uranium was significantly lower than that of conventional mining, however, the footprints of copper and gold were not much less compared with conventional mining methods. This is due to the lower ore grade of ISL deposits and recovery compared with high ore grades and recovery of conventional technology. Additionally, the use of large amount of electricity for pumping in case of ISL contributes to this result. The electricity consumed in pumping leaching solutions was by far the greatest contributor to the well-field related activities associated with ISL of uranium, gold and copper. The main strategy to reduce the GHG footprint of ISL mining should be to use electricity derived from low emission sources. In particular, renewable sources such as solar would be suitable for ISL as these operations are typically in remote locations with smaller deposits compared with conventional mining sites.

Abstract: More than 4,000 sandstone-hosted uranium occurrences host over 1.2 billion pounds of mined and in situ U3O8 throughout the Colorado Plateau. Most of the resources are in two distinct mineral systems with deposits hosted in the Triassic Chinle and Jurassic Morrison Formations. In the Chinle mineral system, base metal sulfides typically accompany mineralization. The Morrison mineral system is characterized by V/U ratios up to 20. The uranium source was likely volcanic ash preserved as bentonitic mudstones in the Brushy Basin Member of the Morrison Formation, and lithic volcanic clasts, ash shards, and bentonitic clay in the lower part of the Chinle Formation. Vanadium originated from two possible sources: iron–titanium oxides that are extensively altered in bleached rock near deposits or from similar minerals in variably bleached red beds interbedded with and beneath the Morrison. In Chinle-hosted deposits, in addition to volcanic ash, a contributing source of both vanadium and uranium is proposed here for the first time to be underlying red beds in the Moenkopi and Cutler Formations that have undergone a cycle of reddening-bleaching-reoxidation. Transport in both systems was likely in groundwater through the more permeable sandstones and conglomerate units. The association of uranium minerals with carbonate and more rarely apatite, suggests that transport of uranium was as a carbonate or phosphate complex. The first comprehensive examination of paleoclimate, paleotopography, and subsurface structure of aquifers coupled with analysis of the geochronology of deposits suggests that that there were distinct pulses of uranium mineralization/redistribution during the period from about 259 Ma to 12 Ma when oxidized mineralizing fluids were intermittently rejuvenated in the Plateau in response to changes in tectonic regime and climate. Multiple lines of evidence indicate that deposits formed at ambient temperatures of about 25 °C to no greater than about 140 °C. In both systems, deposits formed where groundwater flow slowed and was subject to evaporative concentration. Stagnant conditions allowed for prolonged interaction of U- and V-enriched groundwater with ferrous iron-bearing reductants, such as illite and iron–titanium oxides, and more rarely organic material such as plant debris. Paragenetically late in the sequence, reducing fluids introduced additional organic matter to some deposits. Reducing fluids and introduced organic matter (now amorphous and altered by radiolysis) may originate from regional petroleum systems where peak oil and gas generation was from ∼ 82 to ∼ 5 Ma. Our novel analysis indicates that these reducing fluids bleached rock and protected affected deposits from remobilization during exposure and weathering that followed uplift of the Plateau (∼80 to 40 Ma).

Abstract: Uranium reserve estimates in ore deposits can be significantly impacted by 226Ra/238U disequilibria arising from the differential mobility of uranium and radium during groundwater transport. 1D reactive transport models were developed to investigate the long-term effects of retention processes (UO2(am) precipitation, U(VI) and Ra sorption on smectite, Ra co-precipitation with barite) on the repartitioning of 238U and 226Ra during formation of roll-front type deposits. Analytical solutions to radioactive decay chains were used in complement to examine the influence of geochemical parameters, including fluid 234U/238U activity ratios and α-recoil loss, on 226Ra/238U disequilibria in uranium ores. Model results demonstrate that smectite and barite can produce 226Ra/238U ratios \textgreater1 at low uranium contents and may explain 226Ra/238U disequilibria occurring in altered rock up- and downstream of roll-front deposits. The capacity of these phases to take up Ra and generate 226Ra/238U disequilibria depends on both mineral contents and groundwater compositions, and is thus expected to be site-specific. Simulations of ore deposits that advance downstream with time demonstrate the formation of stronger 226Ra/238U disequilibria, as expected, in the downgradient side or nose of the ore, reflecting both younger mineralization ages and the presence of active uranium precipitation. Whether disequilibria are positive or negative with respect to secular equilibrium, however, depends on the 234U/238U activity ratio in the fluid from which uranium minerals precipitate. Smaller hydraulic conductivities are shown to generate a narrower range in 226Ra/238U activity ratios with distance, and may explain the occurrence of disequilibria in the limb ore that are less pronounced than those in the nose. Furthermore, the ability of α-recoil loss to decrease 226Ra/238U activity ratios at secular equilibrium may account for negative disequilibria in high grade ores. The South Tortkuduk uranium deposits (Kazakhstan) are subsequently used as a case study to identify the processes and parameters that may contribute to 226Ra/238U disequilibria at this site. Variations in multiple parameters, including clay contents, barite contents, and mineralization ages, are found to reproduce measured 226Ra/238U activity ratios in the roll-front ore. Prioritization of these parameters will necessitate field measurements targeting both groundwater fluids and the host rock. Results from this study will ultimately aid geologists in building appropriate hydrogeochemical data sets to more efficiently locate and exploit uranium ore deposits.

Abstract: Numerous groundwater analyses from the crystalline bedrock in the Forsmark area have been performed between 2002 and 2019, together with thorough geological, geophysical, and hydrogeological studies, within the site investigations carried out by the Swedish Nuclear Fuel and Waste Management Company. The groundwater samples have been taken from boreholes down to ≈ 1000 m and the analysis include major- and trace-elements, stable and radiogenic isotopes, gases and microbes. The chemical and isotopic composition of these groundwaters evidences the presence of non-marine brackish to saline groundwaters with very long residence times (many hundreds of thousands of years) and a series of complex mixing events resulting from the recharge of different waters over time: glacial meltwaters, probably from different glaciations of which the latest culminated some 20,000 years ago, and marine waters from the Baltic starting some 7000 years ago. Later, meteoric water and present Baltic Sea water have recharged in different parts of the upper 100 m. These mixing events have also triggered chemical and microbial reactions that have conditioned some of the important groundwater parameters and, together with the structural complexity of the area, they have promoted a heterogeneous distribution of groundwater compositions in the bedrock. Due to these evident differences in chemistry, residence time and origin of the groundwater, several groundwater types were defined in order to facilitate the visualisation and communication. The differentiation (linked to the paleohydrological history of the area) was based on Cl concentration, Cl/Mg ratio (marine component), and δ18O value (glacial component). The work presented in this paper increases the understanding of the groundwater evolution in fractured and compartmentalised aquifers where mixing processes are the most important mechanisms. The model proposed to characterise the present groundwater system of the Forsmark area will also help to predict the future hydrogeochemical behaviour of the groundwater system after the construction of the repositories for the nuclear wastes.

Abstract: Paleohydrological data from the African tropics and subtropics, including lake, groundwater and speleothem records, are reviewed to show how environments and climates from both hemispheres are inter-related. Although orbitally induced changes in the monsoon strength account for a large part of long-term climatic changes in tropical Africa, the Late Pleistocene–Holocene hydrological fluctuations rather appear to have been a series of abrupt events that reflect complex interactions between orbital forcing, atmosphere, ocean and land surface conditions. During the Last Glacial Maximum (23–18ka BP), most records indicate that generally dry conditions have prevailed in both hemispheres, associated with lower tropical land- and sea-surface temperatures. This agrees with simulations using coupled ocean–atmosphere models, which predict cooling and reduced summer precipitation in tropical Africa; the global hydrological cycle was weaker than today when the extent of large polar ice-sheets and sea-ice was a prominent forcing factor of the Earth’s climate. Glacial-interglacial climatic changes started early: a first wetting/warming phase at ca. 17–16ka BP took place during a period of rapid temperature increase in Antarctica. Next, two drastic arid-humid transitions in equatorial and northern Africa occurred around 15–14.5ka BP and 11.5–11ka BP. Both are thought to match the major Greenland warming events, in concert with the switching of the oceanic thermohaline circulation to modern mode. However, part of the climatic signal after 15 ka BP also seems related to the Antarctica climate. During the Holocene, Africa has also experienced rapid hydrological fluctuations of dramatic magnitude compared to the climatic changes at high latitudes. In particular, major dry spells occurred around 8.4–8ka and 4.2–4ka BP in the northern monsoon domain. Comparison with other parts of the world indicates that these events have a worldwide distribution but different regional expressions. In the absence of large polar ice sheets, changes in the continental hydrological cycles in the tropics may have a significant impact on the global climate system. Climate information gathered here allows to identify geographical and methodological gaps, and raise some scientific questions that remain to be solved to better understand how the tropics respond to changes in major climate-forcing factors, and how they influence climate globally.