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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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Title |
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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Year |
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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Abstract |
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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Li, J.; Pang, Z.; Liu, Y.; Hu, S.; Jiang, W.; Tian, L.; Yang, G.; Jiang, Y.; Jiao, X.; Tian, J. |
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Title |
Changes in groundwater dynamics and geochemical evolution induced by drainage reorganization: Evidence from 81Kr and 36Cl dating of geothermal water in the Weihe Basin of China |
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Journal Article |
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Year |
2023 |
Publication |
Earth and Planetary Science Letters |
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Volume |
623 |
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Pages |
118425 |
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Kr dating, Cl dating, Geothermal water, Groundwater dynamics, Weihe basin |
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81Kr and 36Cl can both be used to date groundwater beyond the dating range of 14C. 81Kr usually provides reliable groundwater ages because it has uniform initial distribution and negligible subsurface generation, while 36Cl is commonly influenced by subsurface sources or “dead” chloride dissolution. Therefore, the combined use of 81Kr and 36Cl could provide clues on the evolution history of groundwater. In the present study, we performed 36Cl and 81Kr dating of geothermal water in Weihe Basin of China and interpreted the possible cause of disagreement. Two distinct water masses were identified with distinctive isotopic signals: groundwater with significant δ18O shifts (up to −2.0‰), dissolved dead Cl and ages < 1.0 Ma (Cluster A), and older water with little δ18O shifts, negligible dissolved Cl and ages >1.0 Ma (Cluster B). The results confirm the eastward flow path of Cluster B to the Ancient Sanmen Lake with an increasing trend of Cl concentration and age. Modern recharge from the mountains flows to the basin center with intense interaction between water and carbonate under respective reservoir temperatures (100 ∼ 130 °C). These waters flow through the saline stratum emerging from the spillover of the Ancient Sanmen Lake, resulting in higher dead Cl dissolution. A significant linear relationship is observed with the older end-member of ∼1.3Ma under the topographically-driven faster circulation effect. 81Kr ages seem to support the hypothesis that the birth of the modern Yellow River was at about 1.0–1.3 Ma. We inferred the drainage reorganization from the Ancient Sanmen Lake to the modern Yellow River since the Mid-Pleistocene Transition induced the change in groundwater dynamics as well as its chemical evolution. The excavation of the Ancient Sanmen Lake and the accentuated incision of the Weihe River induced groundwater gradient, and therefore the recharge from precipitation from both slopes of the Qinling Mountains in the south and the Beishan Mountains in the north. Our results highlight the effects of dead Cl on 36Cl dating and demonstrate the significant impact of catchment reorganization on groundwater dynamics and its chemistry. |
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0012-821x |
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THL @ christoph.kuells @ Li2023118425 |
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212 |
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Chase, B.M.; Meadows, M.E. |
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Title |
Late Quaternary dynamics of southern Africa’s winter rainfall zone |
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Journal Article |
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Year |
2007 |
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Earth-Science Reviews |
Abbreviated Journal |
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84 |
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3 |
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103-138 |
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Last Glacial Maximum, palaeoenvironment, Quaternary, southern Africa, westerlies, winter rainfall zone |
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Variations in the nature and extent of southern Africa’s winter rainfall zone (WRZ) have the potential to provide important information concerning the nature of long-term climate change at both regional and hemispheric scales. Positioned at the interface between tropical and temperate systems, southern Africa’s climate is influenced by shifts in the Intertropical Convergence Zone, the westerlies, and the development and position of continental and oceanic anticyclones. Over the last glacial–interglacial cycle substantial changes in the amount and seasonality of precipitation across the subcontinent have been linked to the relative dominance of these systems. Central to this discussion has been the extent to which the region’s glacial climates would have been affected by expansions of Antarctic sea-ice, equatorward migrations of the westerlies, more frequent/intense winter storms and an expanded WRZ. This paper reviews the developing body of evidence pertaining to shifts in the WRZ, and the evolution of ideas that have been presented to explain the patterns observed. Dividing the region into three separate axes, along the western and southern margins of the continent and across the interior into the Karoo and the Kalahari, a range of evidence from both terrestrial sites and marine cores is considered, and potential expansions of the WRZ expansions are explored. Despite the limitations of many of the region’s proxy records, a coherent pattern has begun to develop of a significantly expanded WRZ during phases of the last glacial period, with the best-documented being between 32–17 ka. While more detailed inferences will require the recovery and analysis of longer and better-dated records, this synthesis provides a new baseline for further research in this key region. |
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0012-8252 |
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THL @ christoph.kuells @ chase_late_2007 |
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102 |
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Orloff, K.G.; Mistry, K.; Charp, P.; Metcalf, S.; Marino, R.; Shelly, T.; Melaro, E.; Donohoe, A.M.; Jones, R.L. |
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Title |
Human exposure to uranium in groundwater |
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Journal Article |
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Year |
2004 |
Publication |
Environmental Research |
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94 |
Issue |
3 |
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319-326 |
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Groundwater, Human exposure, Uranium, Urine |
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High concentrations of uranium (mean=620μg/L) were detected in water samples collected from private wells in a residential community. Based on isotopic analyses, the source of the uranium contamination appeared to be from naturally occurring geological deposits. In homes where well water concentrations of uranium exceeded the drinking water standard, the residents were advised to use an alternate water source for potable purposes. Several months after the residents had stopped drinking the water, urine samples were collected and tested for uranium. Elevated concentrations of uranium (mean=0.40μg/g creatinine) were detected in urine samples, and 85 percent of the urine uranium concentrations exceeded the 95th percentile concentration of a national reference population. Urine uranium concentrations were positively correlated with water uranium concentrations, but not with the participants’ ages or how long they had been drinking the water. Six months later, a second urine sample was collected and tested for uranium. Urine uranium concentrations decreased in most (63 percent) of the people. In those people with the highest initial urine uranium concentrations, the urine levels decreased an average of 78 percent. However, urine uranium concentrations remained elevated (mean=0.27μg/g), and 87 percent of the urine uranium concentrations exceeded the 95th percentile concentration of the reference population. The results of this investigation demonstrated that after long-term ingestion of uranium in drinking water, elevated concentrations of uranium in urine could be detected up to 10 months after exposure had stopped. |
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0013-9351 |
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THL @ christoph.kuells @ orloff_human_2004 |
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136 |
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Strandmann, P.A.E.P. von; Reynolds, B.C.; Porcelli, D.; James, R.H.; Calsteren, P. van; Baskaran, M.; Burton, K.W. |
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Assessing continental weathering rates and actinide transport in the Great Artesian Basin |
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Journal Article |
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2006 |
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Geochimica et Cosmochimica Acta |
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70 |
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18, Supplement |
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497 |
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0016-7037 |
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THL @ christoph.kuells @ strandmann_assessing_2006 |
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116 |
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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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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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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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Journal Article |
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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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0016-7037 |
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THL @ christoph.kuells @ ingham_combined_2014 |
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188 |
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Lightfoot, D.R. |
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Moroccan khettara: Traditional irrigation and progressive desiccation |
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Journal Article |
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1996 |
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Geoforum |
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27 |
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2 |
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261-273 |
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A 300 km network of khettara (qanat) subsurface irrigation channels was excavated in the Tafilalt basin beginning in the late 14th century. More than 75 of these chains provided perennial water following the breakup of the ancient city of Sijilmassa. Khettara continued to function for much of the northern oasis until the early 1970s, when new technologies and government policies forced changes. Data on origins, maintenance, and current use were collected from archival sources, aerial photographs, Landsat imagery, and from interviews. Insufficient water resources and unsustainable practices have dramatically lowered the water table, drying up khettara. This has resulted in a loss of local control over water resources, abandonment of a sustainable irrigation system, and progressive desiccation. |
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0016-7185 |
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THL @ christoph.kuells @ Lightfoot1996261 |
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257 |
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Rooyen, J.D. van; Watson, A.W.; Miller, J.A. |
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Using tritium and radiocarbon activities to constrain regional modern and fossil groundwater mixing in Southern Africa |
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Journal Article |
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2022 |
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Journal of Hydrology |
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614 |
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128570 |
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Radiocarbon, Residence time, SADC, Tritium |
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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. |
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0022-1694 |
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THL @ christoph.kuells @ rooyen_using_2022 |
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94 |
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Heaton, T.H.E.; Talma, A.S.; Vogel, J.C. |
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Origin and history of nitrate in confined groundwater in the western Kalahari |
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Journal Article |
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1983 |
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Journal of Hydrology |
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62 |
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1 |
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243-262 |
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Data are presented for nitrate, dinitrogen and argon concentrations and 15N14N ratios in groundwater, with radiocarbon ages up to 40,000 yr. for three confined sandstone aquifers in the western Kalahari of South West Africa/Namibia. The nitrate is probably generated within the soil of the recharge areas, and its production rate during the period 3000-40,000 B.P. has remained between 0.5 and 1.6 meq NO−3l−1 of recharge water, with ° 15N between + 4 and + 8‰. Variations in the amount of nitrate and of “excess air” in groundwater recharge are found, and can only reflect changes in the environmental conditions during recharge. They must therefore be caused by the climatic changes that have taken place during the past 25,000 yr. |
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0022-1694 |
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THL @ christoph.kuells @ heaton_origin_1983 |
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95 |
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