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Robin, V.; Beaufort, D.; Tertre, E.; Reinholdt, M.; Fromaget, M.; Forestier, S.; Boissezon, H. de; Descostes, M. |
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Title |
Fate of dioctahedral smectites in uranium roll front deposits exploited by acidic In Situ Recovery (ISR) solutions |
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Journal Article |
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Year |
2020 |
Publication |
Applied Clay Science |
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187 |
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105484 |
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Dissolution, In situ recovery, Ion exchange, Post mining, Remediation, Smectite |
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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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0169-1317 |
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THL @ christoph.kuells @ robin_fate_2020 |
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179 |
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Grozeva, N.G.; Radwan, J.; Beaucaire, C.; Descostes, M. |
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Title |
Reactive transport modeling of U and Ra mobility in roll-front uranium deposits: Parameters influencing 226Ra/238U disequilibria |
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Journal Article |
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Year |
2022 |
Publication |
Journal of Geochemical Exploration |
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Volume |
236 |
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106961 |
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Ra/U, Radioactive disequilibria, Radium, Reactive transport modeling, Roll-front uranium deposit |
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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. |
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0375-6742 |
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THL @ christoph.kuells @ grozeva_reactive_2022 |
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180 |
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Boulesteix, T.; Cathelineau, M.; Deloule, E.; Brouand, M.; Toubon, H.; Lach, P.; Fiet, N. |
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Title |
Ilmenites and their alteration products, sinkholes for uranium and radium in roll-front deposits after the example of South Tortkuduk (Kazakhstan) |
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Journal Article |
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Year |
2019 |
Publication |
Journal of Geochemical Exploration |
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206 |
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106343 |
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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. |
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THL @ christoph.kuells @ boulesteix_ilmenites_2019 |
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181 |
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Lach, P.; Cathelineau, M.; Brouand, M.; Fiet, N. |
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Title |
In-situ Isotopic and Chemical Study of Pyrite from Chu-Sarysu (Kazakhstan) Roll-front Uranium Deposit |
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Journal Article |
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Year |
2015 |
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Procedia Earth and Planetary Science |
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13 |
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207-210 |
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LA-ICP-MS, pyrite, roll-front, SIMS, sulfur isotopy, traces elements, uranium |
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Pyrite is common in roll-front type uranium deposit in Chu-sarysu basin, Kazakhstan. Combined in-situ microstructural, isotopic and chemical analysis of pyrite indicates variation in precipitation conditions and in fluid composition. Broad-scale δ34S heterogeneity indicates a complex multi-facet evolution. First generation authigenic framboïdal aggregates are biogenic as demonstrated by the lowest δ34S values of -48‰ to -28‰. The latest generation pyrites are probably hydrothermal with greater δ34S variation (-30‰ to +12‰). This hydrothermal pyrite commonly displays variable enrichment of several trace elements especially As, Co and Ni. Strong variation in δ34S values and variable trace element enrichment is interpreted in terms of continuous variations in fluid composition. |
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1878-5220 |
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THL @ christoph.kuells @ lach_-situ_2015 |
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182 |
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Etschmann, B.; Liu, W.; Li, K.; Dai, S.; Reith, F.; Falconer, D.; Kerr, G.; Paterson, D.; Howard, D.; Kappen, P.; Wykes, J.; Brugger, J. |
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Enrichment of germanium and associated arsenic and tungsten in coal and roll-front uranium deposits |
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Journal Article |
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2017 |
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Chemical Geology |
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463 |
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29-49 |
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Arsenic, Coal, EXAFS and XANES, germanium, Hydrothermal fluids, Metallogenesis, Speciation, Tungsten |
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Most of the World’s germanium (Ge) is mined from Ge-rich lignite, where it is commonly associated with elevated arsenic (As), tungsten (W) and beryllium (Be) contents. Over the past decade, new evidence showing that World-class Ge deposits result from the interaction of hydrothermal fluids with organic matter in coal seams has emerged. Yet, the chemical state of Ge and associated metals in lignite remains poorly understood. We used Mega-pixel Synchrotron X-ray Fluorescence (MSXRF), X-ray Absorption Near Edge Structure (XANES) and Extended X-ray Absorption Fine Structure (EXAFS) to characterize the oxidation states and chemical bonding environment of Ge, As, and W in two world-class Mesozoic Ge-in-lignite deposits (Lincang, Yunnan, southwestern China; Wulantuga, Inner Mongolia, northeastern China); in lignite-bearing uranium (U) ores from the Beverley deposit (South Australia) hosted in Eocene sandstones; and in lignite and preserved wood in late Oligocene-Miocene fluviatile sediments (Gore, Southland, New Zealand). The aim was to improve our understanding of the enrichment mechanism of Ge in lignite and better evaluate the environmental mobility of Ge and some of the associated metals (specifically As and W) in lignite ores. In all samples, chemical maps show that Ge is distributed homogeneously (down to 2μm) within the organic matter. XANES and EXAFS data show that Ge exists in the tetravalent oxidation state and in a distorted octahedral coordination with O, consistent with complexing of Ge by organic ligands. In some pyrite-bearing samples, a minor fraction of Ge is also present as Ge(IV) in association with pyrite. In contrast, As displays a more complex speciation pattern, sometimes even in a single sample, including As(III), As(V), and As(−I/+II) in solid solution in sulfides. Arsenic in sulfides occurs in anionic and cationic forms, i.e., it shows both the common substitution for S22− and the substitution for Fe recently discovered in some hydrothermal pyrites. Tungsten was present as W(VI) in distorted octahedral (3+3) coordination. The EXAFS data confirm the absence or minor contribution of individual W-rich minerals such as scheelite or ferberite to W mass balance in the studied samples. These data show that Ge, W, and probably some As are scavenged via formation of insoluble, oxygen-bridged metal organic complexes in lignite. Destruction of the organic ligands responsible for fixing Ge and W (As) in these lignites is required for liberating the metals, e.g. from waste materials. Geochemical modelling suggests that Ge, W, Be and As all can be extracted from granitic rocks by dilute, low temperature hydrothermal fluids. Germanium is transported mainly as the tetrahedral Ge(OH)4(aq) complex, but fixed as an octahedral oxy-bridged organic complex. The same situation is valid for W, which is transported at the tetrahedral tungstate ion, but most likely scavenged via formation of a 6-coordinated metal-organic species. The Ge-Be-W±As association in Ge-rich coals reflects the source of the metals as well as related scavenging mechanisms. |
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0009-2541 |
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THL @ christoph.kuells @ etschmann_enrichment_2017 |
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183 |
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Hebert, B.; Baron, F.; Robin, V.; Lelievre, K.; Dacheux, N.; Szenknect, S.; Mesbah, A.; Pouradier, A.; Jikibayev, R.; Roy, R.; Beaufort, D. |
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Quantification of coffinite (USiO4) in roll-front uranium deposits using visible to near infrared (Vis-NIR) portable field spectroscopy |
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Journal Article |
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2019 |
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Journal of Geochemical Exploration |
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199 |
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53-59 |
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Coffinite, Mineral quantification, Near infrared, Ore exploration, Portable field spectroscopy, Roll-front deposits |
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Coffinite (USiO4) is a common uranium-bearing mineral of roll-front uranium deposits. This mineral can be identified by the visible near infrared (Vis-NIR) portable field spectrometers used in mining exploration. However, due to the low detection limits and associated errors, the quantification of coffinite abundance in the mineralized sandstones or sandy sediments of roll-front uranium deposits using Vis-NIR spectrometry requires a specific methodological development. In this study, the 1135 nm absorption band area is used to quantify the abundance of coffinite. This absorption feature does not interfere with NIR absorption bands of any other minerals present in natural sands or sandstones of uranium roll-front deposits. The correlation between the 1135 nm band area and coffinite content was determined from a series of spectra measured from prepared mineral mixtures. The samples were prepared with a range of weighted amounts of arenitic sands and synthetic coffinite simulating the range of uranium concentration encountered in roll-front uranium deposits. The methodology presented in this study provides the quantification of the coffinite content present in sands between 0.03 wt% to 1 wt% coffinite with a detection limit as low as 0.005 wt%. The integrated area of the 1135 nm band is positively correlated with the coffinite content of the sand in this range, showing that the method is efficient to quantify coffinite concentrations typical of roll-front uranium deposits. The regression equation defined in this study was then used as a reference to predict the amount of natural coffinite in a set of mineralized samples from the Tortkuduk uranium roll-front deposit (South Kazakhstan). |
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0375-6742 |
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THL @ christoph.kuells @ hebert_quantification_2019 |
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184 |
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Bonnetti, C.; Zhou, L.; Riegler, T.; Brugger, J.; Fairclough, M. |
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Large S isotope and trace element fractionations in pyrite of uranium roll front systems result from internally-driven biogeochemical cycle |
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Journal Article |
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2020 |
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Geochimica et Cosmochimica Acta |
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282 |
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113-132 |
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Activity cycle, Pyrite composition, Roll front uranium deposits, S isotope and trace element fractionation |
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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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0016-7037 |
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THL @ christoph.kuells @ bonnetti_large_2020 |
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185 |
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Min, M.; Xu, H.; Chen, J.; Fayek, M. |
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Evidence of uranium biomineralization in sandstone-hosted roll-front uranium deposits, northwestern China |
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Journal Article |
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2005 |
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Ore Geology Reviews |
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26 |
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3 |
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198-206 |
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Biomineralization, China, Roll-front uranium deposit, Sandstone |
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We show evidence that the primary uranium minerals, uraninite and coffinite, from high-grade ore samples (U3O8\textgreater0.3%) in the Wuyiyi, Wuyier, and Wuyisan sandstone-hosted roll-front uranium deposits, Xinjiang, northwestern China were biogenically precipitated and psuedomorphically replace fungi and bacteria. Uranium (VI), which was the sole electron acceptor, was likely to have been enzymically reduced. Post-mortem accumulation of uranium may have also occurred through physio-chemical interaction between uranium and negatively-charged cellular sites, and inorganic adsorption or precipitation reactions. These results suggest that microorganisms may have played a key role in formation of the sandstone- or roll-type uranium deposits, which are among the most economically significant uranium deposits in the world. |
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0169-1368 |
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THL @ christoph.kuells @ min_evidence_2005 |
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186 |
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Li, X.; Shen, K.; Li, Q.; Deng, Y.; Zhu, P.; Wang, D. |
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Roll-over behavior in current-voltage curve introduced by an energy barrier at the front contact in thin film CdTe solar cell |
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Journal Article |
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2018 |
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Solar Energy |
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165 |
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27-34 |
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AlO HRT layer, Band alignment, CdTe solar cell, Roll-over behavior |
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Roll-over phenomenon in the current–voltage (J–V) curve is often observed in a CdTe thin film solar cell. The roll-over phenomenon, which is occurred near the open-circuit voltage in a light J–V curve, is due to Schottky energy barrier formed at the CdTe/metal interface in a CdTe solar cell back contact. In this study we report a J–V roll-over phenomenon which is induced by an energy barrier at the front contact of a CdTe solar cell. Two kinds of oxides, namely, Al2O3 and SnO2, were deposited as high-resistance transparent (HRT) layer between the window layer CdS and the fluorine doped tin oxide (FTO) front electrode in CdTe solar cells. These two oxides present much different electronic band alignment with FTO and CdS. SnO2 formed almost no energy barrier with CdS, this allowed smooth transport for photo-generated electrons from CdTe to CdS and FTO. However, Al2O3 formed a high energy barrier with CdS. The rather high energy barrier with a value of 3.43 eV at the CdS/Al2O3 interface induced a J–V roll-over phenomenon in a CdTe thin film solar cell, which dramatically led to a quick decrease for the cell device efficiency. The electron transport at the FTO/Al2O3/CdS interface is governed by tunneling effect. The results presented in this study demonstrate that the band structure at the front electrode plays an important role for the performance of a CdTe thin film solar cell. |
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THL @ christoph.kuells @ li_roll-over_2018 |
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187 |
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Ingham, E.S.; Cook, N.J.; Cliff, J.; Ciobanu, C.L.; Huddleston, A. |
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A combined chemical, isotopic and microstructural study of pyrite from roll-front uranium deposits, Lake Eyre Basin, South Australia |
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2014 |
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Geochimica et Cosmochimica Acta |
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125 |
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440-465 |
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The common sulfide mineral pyrite is abundant throughout sedimentary uranium systems at Pepegoona, Pepegoona West and Pannikan, Lake Eyre Basin, South Australia. Combined chemical, isotopic and microstructural analysis of pyrite indicates variation in fluid composition, sulfur source and precipitation conditions during a protracted mineralization event. The results show the significant role played by pyrite as a metal scavenger and monitor of fluid changes in low-temperature hydrothermal systems. In-situ micrometer-scale sulfur isotope analyses of pyrite demonstrated broad-scale isotopic heterogeneity (δ34S=−43.9 to +32.4‰VCDT), indicative of complex, multi-faceted pyrite evolution, and sulfur derived from more than a single source. Preserved textures support this assertion and indicate a genetic model involving more than one phase of pyrite formation. Authigenic pyrite underwent prolonged evolution and recrystallization, evidenced by a genetic relationship between archetypal framboidal aggregates and pyrite euhedra. Secondary hydrothermal pyrite commonly displays hyper-enrichment of several trace elements (Mn, Co, Ni, As, Se, Mo, Sb, W and Tl) in ore-bearing horizons. Hydrothermal fluids of magmatic and meteoric origins supplied metals to the system but the geochemical signature of pyrite suggests a dominantly granitic source and also the influence of mafic rock types. Irregular variation in δ34S, coupled with oscillatory trace element zonation in secondary pyrite, is interpreted in terms of continuous variations in fluid composition and cycles of diagenetic recrystallization. A late-stage oxidizing fluid may have mobilized selenium from pre-existing pyrite. Subsequent restoration of reduced conditions within the aquifer caused ongoing pyrite re-crystallization and precipitation of selenium as native selenium. These results provide the first qualitative constraints on the formation mechanisms of the uranium deposits at Beverley North. Insights into depositional conditions and sources of both sulfide and uranium mineralization and an improved understanding of pyrite geochemistry can also underpin an effective vector for uranium exploration at Beverley North and other sedimentary systems of the Lake Eyre Basin, as well as in comparable geological environments elsewhere. |
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THL @ christoph.kuells @ ingham_combined_2014 |
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188 |
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