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USGS1988

The aqueous geochemistry of uranium in a drainage containing uraniferous organic-rich sediments, Lake Tahoe area, Nevada, USA

Anomalously uraniferous waters occur in a small (4.2 km2) drainage in the west-central Carson Range, Nevada, on the eastern side of Lake Tahoe. The waters transport uranium from local U-rich soils and bedrock to organic-rich valley-fill sediments where it is concentrated, but weakly bound. The dissolved U and the U that is potentially available from coexisting sediments pose a threat to the quality of drinking water that is taken from the drainage. The U concentration in samples of 6 stream, 11 spring and 7 near-surface waters ranged from <1 to 177 ??g l-1 with an average value of 17 ?? 14 ??g l-1 for stream and spring waters. This value significantly exceeds a reported regional average value of ~5 ??g l-1, and is comparable to proposed maximum contaminant levels of U in drinking water. Calculations that utilize chemical compositions of the waters and thermodynamic data indicate that uranyl-carbonate and uranyl-phosphate complexes are the major inorganic species of dissolved U. In addition, dialysis experiments suggest an association of at least some dissolved U with macromolecular organic matter, particularly in near-surface waters that are in contact with organic-rich sediments. Calculations of the saturation index for uranous and uranyl-bearing minerals indicate that all of the waters are undersaturated with uranium minerals as long as ambient Eh is oxidizing (i.e. > 0.1 V). Possible precipitation of U(IV) minerals is predicted under the more reducing conditions that are particularly likely in near-surface waters, but the inhibitory effects of sluggish kinetics or organic complexing are not considered. These combined results suggest that a process such as adsorption or ion exchange, rather than mineral saturation, is the most probable mechanism for uranium fixation in the sediments. -Authors

Uranium↗

USGS1984

Determination of uranium concentration in water by liquid anion exchange-delayed neutron analysis

Dissolved uranium is selectively removed from 11 of filtered, acidified water using a liquid anion exchange resin (Amberlite LA-1) dissolved in 10 ml of purified kerosene. The organic phase is then analyzed by a standard delayed neutron counting technique. Yields of removed uranium are consistently greater than 90 percent over a measured concentration range of 1.0 to 100 ppb uranium. The absolute detection limit based on 11 of water is 0.06 ppb. Elemental interferences are minimal and the results compare favorably with fluorometric analyses of natural waters.

Journal of Radioanalytical and Nuclear Chemistry↗

USGS1972

A neutron activation analysis procedure for the determination of uranium, thorium and potassium in geologic samples

A neutron activation analysis procedure was developed for the determination of uranium, thorium and potassium in basic and ultrabasic rocks. The three elements are determined in the same 0.5-g sample following a 30-min irradiation in a thermal neutron flux of 2·10 12 n·cm −2 ·sec −1 . Following radiochemical separation, the nuclides 239 U (T=23.5 m), 233 Th (T=22.2 m) and 42 K (T=12.36 h) are measured by β-counting. A computer program is used to resolve the decay curves which are complex owing to contamination and the growth of daughter activities. The method was used to determine uranium, throium and potassium in the U. S. Geological Survey standard rocks DTS-1, PCC-1 and BCR-1. For 0.5-g samples the limits of detection for uranium, throium and potassium are 0.7, 1.0 and 10 ppb, respectively.

Journal of Radioanalytical Chemistry↗

USGS1959

Determination of uranium in zircon

A routine fluorimetric procedure is described for the determination of trace amounts of uranium in zircon. It employs the direct extraction of uranyl nitrate with ethyl acetate using phosphate as a retainer for zirconium. Submicrogram amounts or uranium are separated in the presence of 100,000 times the amount of zirconium. The modified procedure has been worked out using synthetic mixtures of known composition and zircon. Results of analyses have an accuracy of 97–98% of the contained uranium and a standard deviation of less than 2.5%.

Analytica Chimica Acta↗

USGS1969

Dilemma posed by uranium-series dates on archaeologically significant bones from Valsequillo, Puebla, Mexico

In an attempt to date stone artifacts of Early Man excavated from several sites at the Valsequillo Reservoir, a few kilometers south of Puebla, Mexico, Szabo applied the uranium-series method on bone samples known to be either from the same geologic formation as the sites or in direct association with the artifacts. The geologic context of the bones was studied by Malde, and the archaeological sites were excavated by Irwin-Williams. A date determined for bone associated with an artifact (Caulapan sample M-B-6, see below) agrees with a radiocarbon date for fossil mollusks in the same bed and indicates man's presence more than 20 000 years ago. However, some of these bone dates exceed 200 000 years. Because such dates for man in North America conflict with all prior archaeological evidence here and abroad, we are confronted by a dilemna — either to defend the dates against an onslaught of archaeological thought, or to abandon the uranium method in this application as being so much wasted effort. Faced with these equally undesirable alternatives, and unable to decide where the onus fairly lies (if a choice must be made), we give the uranium-series dates as a possible stimulus for further mutual work in isotopic dating of archaeological material. A sample from the Lindenmeier archaeological site north of Fort Collins and another from a Pleistocene terrace along the Arkansas River, both in Colorado, were also dated.

Puebla↗

USGS1969

Loss of uranium from crystallized silicic volcanic rocks

Dense primarily crystallized silicic groundmass material from two welded ash-flow units and one lava flow of Tertiary age from the Western United States contain only 20 to 60 percent of the uranium present in nonhydrated glass from the rock units. These differences reflect loss of uranium from the crystallized specimens, probably as a result of groundwater leaching. It appears likely that most crystallized silicic volcanic rocks have lost comparable amounts of uranium.

Earth and Planetary Science Letters↗

USGS1971

Uranium-series dating of some pleistocene marine deposits in Southern California

Analyses of uranium isotopes and their long-lived daughter products showed evidence of uranium migration in most of the 22 fossil mollusk shell samples from marine terrace deposits in southern California. Two samples, however, remained an ideal closed system as indicated by concordant 230 Th/ 234 U and 231 Pa/ 235 U dates. The closed-system age of the lowest exposed marine terrace deposit along part of the mainland coast of southern California is 69 000 ± 10 000 yr, and correlation of this discontinuous deposit is afforded between the Newport Beach-Laguna Beach area and the Palos Verdes Hills. Some mollusk shell samples were dated by the open-system model; the remaining samples were found to be unsuitable for uranium-series dating.

California↗

USGS1980

U-Pb ages of uraniferous opals and implications for the history of beryllium, fluorine, and uranium mineralization at Spor Mountain, Utah

The U-Pb isotope systematics of uraniferous opals from Spor Mountain, Utah, were investigated to determine the suitability of such material for geochronologic purposes, and to estimate the timing of uranium and associated beryllium and fluorine mineralization. The results indicate that uraniferous opals can approximate a closed system for uranium and uranium daughters, so that dating samples as young as ∼1 m.y. should be possible. In addition, the expected lack of initial 230 Th and 231 Pa in opals permits valuable information on the initial 234 U/ 238 U to be obtained on suitable samples of ≲10 m.y. age. The oldest 207 Pb/ 235 U apparent age observed, 20.8 ± 1m.y., was that of the opal-fluorite core of a nodule from a beryllium deposit in the Spor Mountain Formation. This age is indistinguishable from that of fission-track and K-Ar ages from the host rhyolite, and links the mineralization to the first episode of alkali rhyolite magmatism and related hydrothermal activity at Spor Mountain. Successively younger ages of 13 m.y. and 8–9 m.y. on concentric outer zones of the same nodule indicate that opal formed either episodically or continuously for over 10 m.y. Several samples of both fracture-filling and massive-nodule opal associated with beryllium deposits gave 207 Pb/ 235 U apparent ages of 13–16 m.y., which may reflect a restricted period of mineralization or perhaps an averaging of 21−and<13−m.y. periods of opal growth. Several samples of fracture-filling opal in volcanic rocks as young as 6 m.y. gave 207 Pb/ 235 U ages of 3.4–4.8 m.y. These ages may reflect hot-spring activity after the last major eruption of alkali rhyolite.

Utah↗

USGS1958

Determination of the oxidation state of uranium in apatite and phosphorite deposits

Geological and mineralogical evidence indicate that the uranium present in apatite may proxy for calcium in the mineral structure as U(IV). An experimental investigation was conducted and chemical evidence was obtained that establishes the presence of U(IV) in apatite. The following analytical procedure was developed for the determination of U(IV). Carbonatefluorapatite is dissolved in 1.5 M orthophosphoric acid at a temperature of 5°C or slightly below and fluorapatite is dissolved in cold 1.2 M hydrochloric acid (approximately 5°C) containing 1.5 g of hydroxylamine hydrochloride per 100 ml. Uranium(IV) is precipitated by cupferron using titanium as a carrier. The uranium in the precipitate is separated by use of the ethyl acetate extraction procedure and determined fluorimetrically. The validity and the limitations of the method have been established by spike experiments.

Geochimica et Cosmochimica Acta↗

USGS1975

Uranium determination in natural water by the fissiontrack technique

The fission track technique, utilizing the neutron-induced fission of uranium-235, provides a versatile analytical method for the routine analysis of uranium in liquid samples of natural water. A detector is immersed in the sample and both are irradiated. The fission track density observed in the detector is directly proportional to the uranium concentration. The specific advantages of this technique are: (1) only a small quantity of sample, typically 0.1–1 ml, is needed; (2) no sample concentration is necessary; (3) it is capable of providing analyses with a lower reporting limit of 1 μg per liter; and (4) the actual time spent on an analysis can be only a few minutes. This paper discusses and describes the method.

Journal of Geochemical Exploration↗

USGS1982

Leachability of uranium and other elements from freshly erupted volcanic ash

A study of leaching of freshly erupted basaltic and dacitic air-fall ash and bomb fragment samples, unaffected by rain, shows that glass dissolution is the dominant process by which uranium is initially mobilized from air-fall volcanic ash. Si, Li, and V are also preferentially mobilized by glass dissolution. Gaseous transfer followed by fixation of soluble uranium species on volcanic-ash particles is not an important process affecting uranium mobility. Gaseous transfer, however, may be important in forming water-soluble phases, adsorbed to ash surfaces, enriched in the economically and environmentally important elements Zn, Cu, Cd, Pb, B, F, and Ba. Quick removal of these adsorbed elements by the first exposure of freshly erupted ash to rain and surface water may pose short-term hazards to certain forms of aquatic and terrestrial life. Such rapid release of material may also represent the first step in transportation of economically important elements to environments favorable for precipitation into deposits of commercial interest. Ash samples collected from the active Guatemalan volcanoes Fuego and Pacaya (high-Al basalts) and Santiaguito (hornblende-hypersthene dacite); bomb fragments from Augustine volcano (andesite-dacite), Alaska, and Heimaey (basalt), Vestmann Islands, Iceland; and fragments of "rhyolitic" pumice from various historic eruptions were subjected to three successive leaches with a constant water-to-ash weight ratio of 4:1. The volcanic material was successively leached by: (1) distilled-deionized water (pH = 5.0-5.5) at room temperature for 24 h, which removes water-soluble gases and salts adsorbed on ash surfaces during eruption; (2) dilute HCl solution (pH = 3.5-4.0) at room temperature for 24 h, which continues the attack initiated by the water and also attacks acid-soluble sulfides and oxides; (3) a solution 0.05 M in both Na,CO, and NaHCO, (pH = 9.9) at 80°C for one week, which preferentially dissolves volcanic glass. The first two leaches mimic interaction of ash with rain produced in the vicinity of an active eruption. The third leach accelerates the effect of prolonged contact of volcanic ash with alkaline ground water present during ash diagenesis.

Journal of Volcanology and Geothermal Research↗

USGS2015

Biogeochemical aspects of uranium mineralization, mining, milling, and remediation

Natural uranium (U) occurs as a mixture of three radioactive isotopes: 238 U, 235 U, and 234 U. Only 235 U is fissionable and makes up about 0.7% of natural U, while 238 U is overwhelmingly the most abundant at greater than 99% of the total mass of U. Prior to the 1940s, U was predominantly used as a coloring agent, and U-bearing ores were mined mainly for their radium (Ra) and/or vanadium (V) content; the bulk of the U was discarded with the tailings (Finch et al., 1972). Once nuclear fission was discovered, the economic importance of U increased greatly. The mining and milling of U-bearing ores is the first step in the nuclear fuel cycle, and the contact of residual waste with natural water is a potential source of contamination of U and associated elements to the environment. Uranium is mined by three basic methods: surface (open pit), underground, and solution mining (in situ leaching or in situ recovery), depending on the deposit grade, size, location, geology and economic considerations (Abdelouas, 2006). Solid wastes at U mill tailings (UMT) sites can include both standard tailings (i.e., leached ore rock residues) and solids generated on site by waste treatment processes. The latter can include sludge or “mud” from neutralization of acidic mine/mill effluents, containing Fe and a range of coprecipitated constituents, or barium sulfate precipitates that selectively remove Ra (e.g., Carvalho et al., 2007). In this chapter, we review the hydrometallurgical processes by which U is extracted from ore, the biogeochemical processes that can affect the fate and transport of U and associated elements in the environment, and possible remediation strategies for site closure and aquifer restoration. This paper represents the fourth in a series of review papers from the U.S. Geological Survey (USGS) on geochemical aspects of UMT management that span more than three decades. The first paper (Landa, 1980) in this series is a primer on the nature of tailings and radionuclide mobilization from them. The second paper (Landa, 1999) includes coverage of research carried out under the U.S. Department of Energy’s Uranium Mill Tailings Remedial Action Program (UMTRA). The third paper (Landa, 2004) reflects the increased focus of researchers on biotic effects in UMT environs. This paper expands the focus to U mining, milling, and remedial actions, and includes extensive coverage of the increasingly important alkaline in situ recovery and groundwater restoration.

Applied Geochemistry↗

USGS2021

Terrestrial ecological risk analysis via dietary exposure at uranium mine sites in the Grand Canyon watershed (Arizona, USA)

The U.S. Department of the Interior recently included uranium (U) on a list of mineral commodities that are considered critical to economic and national security. The uses of U for commercial and residential energy production, defense applications, medical device technologies, and energy generation for space vehicles and satellites are known, but the environmental impacts of uranium extraction are not always well quantified. We conducted a screening-level ecological risk analysis based on exposure to mining-related elements via diets and incidental soil ingestion for terrestrial biota to provide context to chemical characterization and exposures at breccia pipe U mines in northern Arizona. Relative risks, calculated as hazard quotients (HQs), were generally low for all biological receptor models. Our models screened for risk to omnivores and insectivores (HQs>1) but not herbivores and carnivores. Uranium was not the driver of ecological risk; arsenic, cadmium, copper, and zinc were of concern for biota consuming ground-dwelling invertebrates. Invertebrate species composition should be considered when applying these models to other mining locations or future sampling at the breccia pipe mine sites. Dietary concentration thresholds (DCTs) were also calculated to understand food concentrations that may lead to ecological risk. The DCTs indicated that critical concentrations were not approached in our model scenarios, as evident in the very low HQs for most models. The DCTs may be used by natural resource and land managers as well as mine operators to screen or monitor for potential risk to terrestrial receptors as mine sites are developed and remediated in the future.

Arizona↗

USGS2006

Processes affecting transport of uranium in a suboxic aquifer

At the Naturita site in Colorado, USA, groundwaters were sampled and analyzed for chemical composition and by culture and culture-independent microbiological techniques. In addition, sediments were extracted with a dilute sodium carbonate solution to determine quantities of labile uranium within the sediments. Samples from the upgradient portion of the contaminated aquifer , where very little dissolved Fe(II) is found in the groundwater, have uranium content that is controlled by U(VI) adsorption and few metal-reducing bacteria are observed. In the extreme downgradient portion of the aquifer, where dissolved Fe(II) is observed, uranium content of the sediments includes significant quantities of reduced U(IV) and diverse populations of Fe(III)-reducing bacteria were present in the subsurface with the potential of reducing U(VI) to U(IV).

Physics and Chemistry of the Earth↗

USGS2002

Determination of uranium in natural waters

The fluorophotometric determination of uranium was studied to develop a procedure applicable to the routine analysis of waters. Three grams of the high carbonate flux are used in a dilution procedure with spiking. Because of the comparatively high reflectivity of this large disk and the low uranium concentration, a correction for nonquenched light is required. A formula is developed to compensate for the effect, an electrical fusion device is described, and the problem of fixing uranium in waters is discussed.

Analytical Chemistry↗

USGS2016

Biogeochemical controls of uranium bioavailability from the dissolved phase in natural freshwaters

To gain insights into the risks associated with uranium (U) mining and processing, we investigated the biogeochemical controls of U bioavailability in the model freshwater species Lymnaea stagnalis (Gastropoda). Bioavailability of dissolved U(VI) was characterized in controlled laboratory experiments over a range of water hardness, pH, and in the presence of complexing ligands in the form of dissolved natural organic matter (DOM). Results show that dissolved U is bioavailable under all the geochemical conditions tested. Uranium uptake rates follow first order kinetics over a range encompassing most environmental concentrations. Uranium uptake rates in L. stagnalis ultimately demonstrate saturation uptake kinetics when exposure concentrations exceed 100 nM, suggesting uptake via a finite number of carriers or ion channels. The lack of a relationship between U uptake rate constants and Ca uptake rates suggest that U does not exclusively use Ca membrane transporters. In general, U bioavailability decreases with increasing pH, increasing Ca and Mg concentrations, and when DOM is present. Competing ions did not affect U uptake rates. Speciation modeling that includes formation constants for U ternary complexes reveals that the aqueous concentration of dicarbonato U species (UO 2 (CO 3 ) 2 –2 ) best predicts U bioavailability to L. stagnalis , challenging the free-ion activity model postulate.

Environmental Science & Technology↗

USGS2011

Quantifying differences in the impact of variable chemistry on equilibrium uranium(VI) adsorption properties of aquifer sediments

Uranium adsorption-desorption on sediment samples collected from the Hanford 300-Area, Richland, WA varied extensively over a range of field-relevant chemical conditions, complicating assessment of possible differences in equilibrium adsorption properties. Adsorption equilibrium was achieved in 500-1000 h although dissolved uranium concentrations increased over thousands of hours owing to changes in aqueous chemical composition driven by sediment-water reactions. A nonelectrostatic surface complexation reaction, >SOH + UO 2 2+ + 2CO 3 2- = >SOUO 2 (CO 3 HCO 3 ) 2- , provided the best fit to experimental data for each sediment sample resulting in a range of conditional equilibrium constants (log K c ) from 21.49 to 21.76. Potential differences in uranium adsorption properties could be assessed in plots based on the generalized mass-action expressions yielding linear trends displaced vertically by differences in log K c values. Using this approach, log K c values for seven sediment samples were not significantly different. However, a significant difference in adsorption properties between one sediment sample and the fines (<0.063 mm) of another could be demonstrated despite the fines requiring a different reaction stoichiometry. Estimates of log K c uncertainty were improved by capturing all data points within experimental errors. The mass-action expression plots demonstrate that applying models outside the range of conditions used in model calibration greatly increases potential errors.

Washington↗

USGS2019

Biota dose assessment of small rodents sampled near breccia pipe uranium mines in the Grand Canyon watershed

The biotic exposure and uptake of radionuclides and potential health effects due to breccia pipe uranium mining in the Grand Canyon watershed are largely unknown. This paper describes the use of the RESRAD-BIOTA dose model to assess exposure of small rodents (n = 11) sampled at three uranium mine sites in different stages of ore production (active and postproduction). Rodent tissue and soil concentrations of naturally occurring uranium (234U, 235U, and 238U), thorium (228Th, 230Th, and 232Th), and radium (226Ra) radioisotopes were used in the dose model. The dose assessment results indicated that the potential internal, external, and total doses to rodents were below the US Department of Energy’s biota dose standard of 1 mGy d−1. As expected, tissue concentrations of 238U, 234U, and 230Th were in approximate equilibrium; however, 226Ra results in tissue were 1.25 to 5.75 times greater than 238U, 234U, and 230Th tissue results for 10 out of 11 samples. Soil at the three sites also displayed 226Ra enrichment, so it is likely that the 226Ra enrichment in the rodents was from soil via typical activities (i.e., burrowing, incidental ingestion, bathing, etc.) or by dietary uptake of translocated 226Ra. The results suggest that 226Ra is more mobile in this environment and bioaccumulates in these rodent species (e.g., in bones via the bloodstream). Internal dose accounting suggests that 226Ra is the radionuclide of most concern for rodent exposure and health.

Grand Canyon↗