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Gardiner, J., Thomas, R. B., Phan, T. T., Stuckman, M., Wang, J., Small, M., et al. (2020). Utilization of produced water baseline as a groundwater monitoring tool at a CO2-EOR site in the Permian Basin, Texas, USA. Applied Geochemistry, 121, 104688.
Abstract: Carbon dioxide (CO2) enhanced oil recovery (EOR) provides a pathway for economic reuse and storage of CO2, a greenhouse gas. One challenge with this practice is ensuring CO2 injection does not result in target reservoir fluids migrating into overlying shallow (\textless1000 m) groundwater formations. Effective monitoring for leakage from storage formations could involve measuring sensitive chemical indicators in overlying groundwater units and within the producing formation itself for evidence of deviation from an initial state. In this study, produced waters and overlying groundwaters were monitored over a five-year period to evaluate which geochemical signals may be useful to ensure that oilfield produced waters did not impact overlying groundwaters. During this five-year period, a mature carbonate oil reservoir in the Permian Basin transitioned from a waterflooding operation to a water-alternating-gas injection (WAG), in which the formation was flooded with CO2 and various mixtures of produced water. Significant increases in dissolved inorganic constituents [alkalinity, TDS, Na+, Cl−, SO42−] were observed in produced waters following CO2 injection; however, carbonate reservoir dissolution-precipitation reactions appear to be minimal and injected CO2 appears to be stored via solubility trapping. Although there are statistically significant geochemical variations following CO2 injection, applying isometric log-ratios to certain parameters establishes a narrow range for post-CO2 injection produced waters. This narrow range can be considered a baseline for post-CO2 injection produced waters; this baseline can be utilized to monitor overlying local groundwaters for produced water intrusion. Additionally, certain parameters [Na+, Ca2+, K+, Cl−, alkalinity, and TDS] display large concentration disparities between produced water and overlying groundwaters; these parameters would be sensitive indicators of produced water intrusion into overlying groundwaters.
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Jroundi, F., Descostes, M., Povedano-Priego, C., Sánchez-Castro, I., Suvannagan, V., Grizard, P., et al. (2020). Profiling native aquifer bacteria in a uranium roll-front deposit and their role in biogeochemical cycle dynamics: Insights regarding in situ recovery mining. Science of The Total Environment, 721, 137758.
Abstract: A uranium-mineralized sandy aquifer, planned for mining by means of uranium in situ recovery (U ISR), harbors a reservoir of bacterial life that may influence the biogeochemical cycles surrounding uranium roll-front deposits. Since microorganisms play an important role at all stages of U ISR, a better knowledge of the resident bacteria before any ISR actuations is essential to face environmental quality assessment. The focus here was on the characterization of bacteria residing in an aquifer surrounding a uranium roll-front deposit that forms part of an ISR facility project at Zoovch Ovoo (Mongolia). Water samples were collected following the natural redox zonation inherited in the native aquifer, including the mineralized orebody, as well as compartments located both upstream (oxidized waters) and downstream (reduced waters) of this area. An imposed chemical zonation for all sensitive redox elements through the roll-front system was observed. In addition, high-throughput sequencing data showed that the bacterial community structure was shaped by the redox gradient and oxygen availability. Several interesting bacteria were identified, including sulphate-reducing (e.g. Desulfovibrio, Nitrospira), iron-reducing (e.g. Gallionella, Sideroxydans), iron-oxidizing (e.g. Rhodobacter, Albidiferax, Ferribacterium), and nitrate-reducing bacteria (e.g. Pseudomonas, Aquabacterium), which may also be involved in metal reduction (e.g. Desulfovibrio, Ferribacterium, Pseudomonas, Albidiferax, Caulobacter, Zooglea). Canonical correspondence analysis (CCA) and co-occurrence patterns confirmed strong correlations among the bacterial genera, suggesting either shared/preferred environmental conditions or the performance of similar/complementary functions. As a whole, the bacterial community residing in each aquifer compartment would appear to define an ecologically functional ecosystem, containing suitable microorganisms (e.g. acidophilic bacteria) prone to promote the remediation of the acidified aquifer by natural attenuation. Assessing the composition and structure of the aquifer’s native bacteria is a prerequisite for understanding natural attenuation and predicting the role of bacterial input in improving ISR efficiency.
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Robin, V., Beaufort, D., Tertre, E., Reinholdt, M., Fromaget, M., Forestier, S., et al. (2020). Fate of dioctahedral smectites in uranium roll front deposits exploited by acidic In Situ Recovery (ISR) solutions. Applied Clay Science, 187, 105484.
Abstract: In Situ Recovery (ISR) is the most important process of uranium production in the world (50%). It consists of an injection of a leaching solution into a permeable mineralized aquifer (sandstone), pumping of the solution after dissolution of the ore minerals and recovery of the uranium from the pregnant solution in a surface plant. In this context, the fate of swelling clay minerals such as smectites is of main importance due to their role in the mobility of cationic elements by diverse geochemical processes such as ion-exchange reactions or dissolution. The present study details analysis of dioctahedral smectites before and after in-situ leaching by acidic (H2SO4) ISR solutions. Samples were collected from two sedimentary basins hosting some of the main uranium roll front deposits exploited by acidic ISR (Tortkuduk deposit, Shu-Saryssu basin, Kazakhstan, and Dulaan Uul and Zoovch Ovoo deposits, Sainshand basin, Mongolia). Scanning Electron Microscope and X-Ray Diffraction analysis revealed that dioctahedral smectite is a ubiquitous mineral in all analyzed samples, before and after acidification, and revealed a difference of crystal chemistry of the smectites between deposits of Kazakhstan (beidellite type) and Mongolia (montmorillonite type). Chemical analysis and semi-quantification of the smectites before and after acidification also revealed a difference in chemical reactivity, with a higher dissolution of montmorillonite layers compared to beidellite ones, and the importance of ion-exchange reactions. These findings are consistent with literature data obtained on model systems. The persistence of dioctahedral smectites after several years of acidification is crucial for the understanding of geochemical processes during uranium production or remediation of the aquifers. Finally, based on the analysis of samples from U-deposits hosted in both sedimentary basins, a schematic model of the impact of acid solutions on dioctahedral smectite was proposed.
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Bonnetti, C., Zhou, L., Riegler, T., Brugger, J., & Fairclough, M. (2020). Large S isotope and trace element fractionations in pyrite of uranium roll front systems result from internally-driven biogeochemical cycle. Geochimica et Cosmochimica Acta, 282, 113–132.
Abstract: Complex pyrite textures associated with large changes in isotopic and trace element compositions are routinely assumed to be indicative of multi-faceted processes involving multiple fluid and sulfur sources. We propose that the features of ore-stage pyrite from roll front deposits across the world, revealed in exquisite detail via high-resolution trace element mapping by LA-ICP-MS, reflect the dynamic internal evolution of the biogeochemical processes responsible for sulfate reduction, rather than externally driven changes in fluid or sulfur sources through time. Upon percolation of oxidizing fluids into the reduced host-sandstones, roll front systems become self-organized, with a systematic reset of their activity cycle after each translation stage of the redox interface down dip of the aquifer. Dominantly reducing conditions at the redox interface favor the formation of biogenic framboidal pyrite (δ34S from −30.5 to −12.5‰) by bacterial sulfate reduction and the genesis of the U mineralization. As the oxidation front advances, oxidation of reduced sulfur minerals induces an increased supply of sulfate and metals in solution to the bacterial sulfate reduction zone that has similarly advanced down the flow gradient. Hence, this stage is marked by increased rates of the bacterial sulfate reduction associated with the crystallization of variably As-Co-Ni-Mo-enriched concentric pyrite (up to 10,000′s of ppm total trace contents) with moderately negative δ34S values (from −13.7 to −7.5‰). A final stage of pyrite cement with low trace element contents and heavier δ34S signature (from −6.9 to +18.8‰) marks the end of the roll front activity cycle and the transition from an open to a predominantly closed system behavior (negligible advection of fresh sulfate). Blocky pyrite cement is formed using the remaining sulfate, which now becomes quickly heavy according to a Rayleigh isotope fractionation process. This ends the cycle by depleting the nutrient supplies for the sulfate-reducing bacteria and cementing pore spaces within the host sandstone, effectively restricting fluid infiltration. This internally-driven roll front activity cycle results in systematic, large S isotope and trace element fractionation. Ultimately, the long-time evolution of the basin and fluid sources control the metal endowment and evolution of the system; these events, however, are unlikely to be preserved by the roll front, as a direct result of its hydrodynamic nature.
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Zhou, Y., Li, G., Xu, L., Liu, J., Sun, Z., & Shi, W. (2020). Uranium recovery from sandstone-type uranium deposit by acid in-situ leaching – an example from the Kujieertai. Hydrometallurgy, 191, 105209.
Abstract: The factors influencing uranium recovery in water-rock systems during acid in-situ leaching (ISL) were studied at the Kujieertai uranium deposit in Xinjiang. Using an ISL unit, a field leach trial (FLT) had been carried out to test the sequential effects of a leaching solution without oxidant (H2SO4 solution 4–8 g/L) and a leaching solution with oxidant (H2SO4 3–7 g/L, and Fe (III) 2–6 g/L). The observation of the leaching process revealed clearly defined stages of uranium release from the solid mineral to solution. Uranium mobilization from solid mineral into solution can be described in four stages. At the beginning of the acid ISL process, there was no oxidant to be added to the leaching solution and the desorption of hexavalent uranyl ions in the open pores, as well as dissolution of hexavalent uranium minerals, led to a short-term peak in the pregnant solution, which happened while pH decreased from about 5.3 to 2.62. Following the depletion of the adsorbed hexavalent uranium and a decline in uranium dissolution intensity, the addition of Fe(III) facilitated the oxidation of tetravalent uranium, which enabled intensive uranium mobilization again. During this process, the dissolution of uranium had a strong positive correlation with the reduction of Fe(III) and Eh in the leach solution. Beside hydrochemical factors, the deportment of uranium was also an important factor affecting uranium recovery. Uranium located in the open pores can be completely exposed to the solution and the mobilization intensity was significantly affected by hydrogeochemical conditions; but the uranium present in microfissures and in the ore matrix could not be fully exposed to the solution, so, their dissolution intensity was primarily controlled by corrosion and permeability of the ore. In general, the hydrogeochemical conditions and the deportment of uranium were the external and internal factors that significantly affected the dissolution and recovery of uranium in the early and middle stages of the FLT. However, in the latest stages, due to uranium depletion, enhancing the chemical potential of the leaching solution, specifically acidity and/or the amount of oxidant, had little improvement on uranium recovery.
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