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Bonnetti, C.; Zhou, L.; Riegler, T.; Brugger, J.; Fairclough, M. |
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Title |
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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Year |
2020 |
Publication  |
Geochimica et Cosmochimica Acta |
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282 |
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113-132 |
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Keywords |
Activity cycle, Pyrite composition, Roll front uranium deposits, S isotope and trace element fractionation |
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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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0016-7037 |
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THL @ christoph.kuells @ bonnetti_large_2020 |
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185 |
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Mahindawansha, A.; Külls, C.; Kraft, P.; Breuer, L. |
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Title |
Investigating unproductive water losses from irrigated agricultural crops in the humid tropics through analyses of stable isotopes of water |
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Journal Article |
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2020 |
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Hydrology and Earth System Sciences |
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24 |
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7 |
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3627-3642 |
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Copernicus GmbH |
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yes |
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THL @ christoph.kuells @ Mahindawansha2020investigating |
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14 |
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Zhou, Y.; Li, G.; Xu, L.; Liu, J.; Sun, Z.; Shi, W. |
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Title |
Uranium recovery from sandstone-type uranium deposit by acid in-situ leaching – an example from the Kujieertai |
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Journal Article |
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2020 |
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Hydrometallurgy |
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191 |
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105209 |
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Acid in-situ leaching, Sandstone-type uranium deposit, Uranium deportment in the ore, Uranium recovery, Water-rock interaction |
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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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0304-386x |
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THL @ christoph.kuells @ zhou_uranium_2020 |
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205 |
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Author |
Pree, T.A.D. |
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Title |
The politics of baselining in the Grants uranium mining district of northwestern New Mexico |
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Journal Article |
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2020 |
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Journal of Environmental Management |
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268 |
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110601 |
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Critical stakeholder analysis, Environmental cleanup, Environmental monitoring, Mining reclamation/remediation/restoration, Politics of baselining |
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During the second half of the twentieth century, northwestern New Mexico served as the primary production site for one of the world’s largest nuclear arsenals. From 1948 to 1970 the “Grants uranium district” provided almost half of the total uranium ore accumulated by the United States federal government for the production of nuclear weapons, in addition to becoming a national source for commercial nuclear energy from the late 1960s to the early 1990s. By the twenty-first century, after a prolonged period of economic decline that began in the late 1970s, all uranium mining and milling in New Mexico had ceased, leaving a legacy of environmental health impacts. What was once referred to as “The Uranium Capital of the World” now encompasses over a thousand abandoned uranium mines and seven massive uranium mill tailings piles, which are associated with airborne and soil contamination as well as groundwater plumes of uranium and other contaminants of concern, in a landscape that has been fractured by underground mine workings and punctured by thousands of exploratory boreholes. This article presents an ethnographic study of the diverse forms of expertise involved in monitoring and managing the mine waste and mill tailings. Drawing from over two years of ethnographic research, I describe the relationship between different stakeholders from local communities, government agencies, and transnational mining corporations as they deliberate about the possibility of cleaning up the former mining district. My thesis is that the possibility of cleaning up the Grants district hinges on the “politics of baselining”—a term I introduce to describe the relationship between stakeholders and their competing environmental models and hydrogeological theories; each accounts for a different geological past prior to mining that can be deemed “natural,” as the background against which to measure the anthropogenic impacts from mining. |
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0301-4797 |
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THL @ christoph.kuells @ pree_politics_2020 |
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151 |
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Gil-Márquez, J.M.; Sültenfuß, J.; Andreo, B.; Mudarra, M. |
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Groundwater dating tools (3H, 3He, 4He, CFC-12, SF6) coupled with hydrochemistry to evaluate the hydrogeological functioning of complex evaporite-karst settings |
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Journal Article |
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2020 |
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Journal of Hydrology |
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580 |
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124263 |
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Groundwater dating, Evaporite karst, Brine spring, Free-shape models |
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The hydrogeological functioning of four different areas in a complex evaporite-karst unit of predominantly aquitard behavior in S Spain was investigated. Environmental dating tracers (3H, 3He, 4He, CFC-12, SF6) and hydrochemical data were determined from spring samples to identify and characterize groundwater flow components of different residence times in the media. Results show a general geochemical evolution pattern, from higher (recharge areas) to lower positions (discharge areas), in which mineralization rises as well as the value of the rCl−/SO42−, evidencing longer water-rock interaction. Ne values show degassing of most of the samples, favored by the high salinity of groundwater and the development of karstification so that the concentration of all the considered gases were corrected according to the difference between the theoretical and the measured Ne. The presence of modern groundwater in every sample was proved by the detection of 3H and CFC-12. At the opposite, the higher amount of radiogenic 4He in most samples also indicates that they have an old component. The 3H/3He dating method does not give reliable ages as a consequence of degassing and the large uncertainty of the 3He/4He ratios of the sources for the radiogenic Helium. The large SF6 concentrations suggest terrigenic production related to halite and dolomite. Binary Mixing and Free Shape Models were created based on 3H and CFC-12 data to interpret the age distribution of the samples. Two parameters (GA50 and >70%) were proposed as an indicator of that distribution, as they provide further information than the mean age. Particularly, GA50 is derived from the median groundwater age and is presented as a new way of interpreting mixed groundwater age data. A greater fraction of old groundwater (3H and CFC-12 free) was identified in discharge areas, while the proportion and estimated infiltration date of the younger fractions in recharge areas were higher and more recent, respectively. The application of different approaches has been useful to corroborate previous theoretical conceptual model proposed for the study area and to test the applicability of the used environmental tracer in dating brine groundwater and karst springs. |
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0022-1694 |
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THL @ christoph.kuells @ Gilmarquez2020124263 |
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213 |
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