Gross-beta activity in ground water: natural sources and artifacts of sampling and laboratory analysis

Gross-beta activity has been used as an indicator of beta-emitting isotopes in water since at least the early 1950s. Originally designed for detection of radioactive releases from nuclear facilities and weapons tests, analysis of gross-beta activity is widely used in studies of naturally occurring radioactivity in ground water. Analyses of about 800 samples from 5 ground-water regions of the United States provide a basis for evaluating the utility of this measurement. The data suggest that measured gross-beta activities are due to (1) long-lived radionuclides in ground water, and (2) ingrowth of beta-emitting radionuclides during holding times between collection of samples and laboratory measurements.Although⁴⁰K and²²⁸Ra appear to be the primary sources of beta activity in ground water, the sum of⁴⁰K plus²²⁸Ra appears to be less than the measured gross-beta activity in most ground-water samples. The difference between the contribution from these radionuclides and gross-beta activity is most pronounced in ground water with gross-beta activities > 10 pCi/L, where these 2 radionuclides account for less than one-half the measured ross-beta activity. One exception is groundwater from the Coastal Plain of New Jersey, where⁴⁰K plus²²⁸Ra generally contribute most of the gross-beta activity. In contrast,⁴⁰K and²²⁸Ra generally contribute most of beta activity in ground water with gross-beta activities < 1 pCi/L.The gross-beta technique does not measure all beta activity in ground water. Although³H contributes beta activity to some ground water, it is driven from the sample before counting and therefore is not detected by gross-beta measurements. Beta-emitting radionuclides with half-lives shorter than a few days can decay to low values between sampling and counting. Although little is known about concentrations of most short-lived beta-emitting radionuclides in environmental ground water (water unaffected by direct releases from nuclear facilities and weapons tests), their activities are expected to be low.Ingrowth of beta-emitting radionuclides during sample holding times can contribute to gross-beta activity, particularly in ground water with gross-beta activities > 10 pCi/L. Ingrowth of beta-emitting progeny of²³⁸U, specifically²³⁴Pa and²³⁴Th, contributes much of the measured gross-beta activity in ground water from 4 of the 5 areas studied. Consequently, gross-beta activity measurements commonly overestimate the abundance of beta-emitting radionuclides actually present in ground water. Differing sample holding times before analysis lead to differing amounts of ingrowth of the two progeny. Therefore, holding times can affect observed gross-beta measurements, particularly in ground water with²³⁸U activities that are moderate to high compared with the activity of⁴⁰K plus²²⁸Ra. Uncertainties associated with counting efficiencies for beta particles with different energies further complicate the interpretation of gross-beta measurements.     

Factors controlling As and U in shallow ground water,southern Carson Desert,Nevada

Unusually high As and U concentrations (>100 μg/L) are widespread in shallow ground water beneath the southern Carson Desert. The high concentrations, which locally exceed 1000 μg/L, are of concern from a human health standpoint because the shallow ground water is used for domestic supply. Possible affects on wildlife are also of concern because the ground water flows into shallow lakes and marshes within wildlife refuges.Arsenic and U concentrations in ground water of the southern Carson Desert appear to be affected by evaporative concentration, redox reactions, and adsorption. The relation of these elements with Cl suggest that most of the high concentrations can be attributed to evaporative concentration of Carson River water, the primary source of recharge.Some ground water contains higher As and U concentrations that cannot be explained by evaporative concentration alone. Oxidation-reduction reactions, involving metal oxides and sedimentary-organic matter, appear to contribute As, U, inorganic C, Fe and Mn to the ground water. Arsenic in Fe-oxide was confirmed by chemical extraction and is consistent with laboratory adsorption studies. Uranium in both sedimentary-organic C and Fe-oxide coatings has been confirmed by fission tracks and petrographic examination.Arsenic concentrations in the ground water and chemical extracts of aquifer sediments are broadly consistent with adsorption as a control on some dissolved As concentrations. An apparent loss of As from some ground water as evaporative concentration proceeds is consistent with adsorption as a control on As. However, evidence for adsorption should be viewed with caution, because the adsorption model used values for the adsorbent that have not been shown to be valid for the aquifer sediments throughout the southern Carson Desert.Hydrologic and geochemical conditions in the Carson Desert are similar to other areas with high As and U concentrations in ground water, including the Salton Sea basin and southern San Joaquin Valley of California. Hydrologic and geochemical conditions that produced some sandstone-type U-ore deposits, including those in the non-marine, closed-basin sediments of the Morrison Formation near Grants, New Mexico, suggest that the Carson Desert may be a modern analog for those systems.     

Ground water geochemistry of 228Ra, 226Ra and 222Rn

²²⁸Ra, ²²⁶Ra, and ²²²Rn activities were determined on over 150 ground water samples collected from drilled, public water supply wells throughout South Carolina. A wide range of aquifer lithologies were sampled including the crystalline rocks of the Piedmont and sedimentary deposits of the Coastal Plain. A significant linear relationship between log ²²⁸Ra and log ²²⁶Ra (n = 182, r = 0.83) was indistinguishable between Piedmont and Coastal Plain ground water. Median ${}^{228}\text{Ra}{}^{226}\text{Ra}$ activity ratios for the Piedmont, 1.2, and Coastal Plain, 1.3, ground water are close to estimated average crustal ${}^{232}\text{Th}{}^{238}\text{U}$ activity ratios of 1.2 to 1.5 corresponding to Th/U weight ratios of 3.5 to 4.5. A linear correlation was also found between log ²²²Rn and log ²²⁶Ra for Piedmont (n = 68, r = 0.62) and Coastal Plain (n = 89, r = 0.64) ground water. However, the median ${}^{222}\text{Rn}{}^{226}\text{Ra}$ activity ratio for Piedmont ground water, 6100, was much higher than for Coastal Plain ground water, 230. Higher excess ²²²Rn activities may be due to greater retention of ²²⁶Ra by the chemically active Piedmont aquifers compared to the more inert sand aquifers sampled in the Coastal Plain. The relationship between log ²²⁸Ra and log ²²⁶Ra was used to predict total Ra (${}^{228}\text{Ra +}{}^{226}\text{Ra}$) distributions in Appalachian and Atlantic and Gulf Coastal Plain ground water. Predictions estimate that 2.4% of Appalachian and 5.3% of Atlantic and Gulf Coastal Plain ground water supplies contain total Ra activities in excess of the 5 pCi/l limit established by the U.S. Environmental Protection Agency. These predictions also indicate that 40–50% of these ground water wells may be overlooked using the presently suggested screening activity of 3.0 pCi/l of ²²⁶Ra for ²²⁸Ra analysis.     

Relationships between radium and radon occurrence and hydrochemistry in fresh groundwater from fractured crystalline rocks, North Carolina (USA)

Naturally-occurring radionuclides (uranium, radium, and radon), major dissolved constituents, and trace elements were investigated in fresh groundwater in 117 wells in fractured crystalline rocks from the Piedmont region (North Carolina, USA). Chemical variations show a general transition between two water types: (1) slightly acidic (pH 5.0–6.0), oxic, low-total dissolved solids (TDS) waters, and (2) near neutral, oxic to anoxic, higher-TDS waters. The uranium, radium, and radon levels in groundwater associated with granite (Rolesville Granite) are systematically higher than other rock types (gneiss, metasedimentary, and metavolcanic rocks). Water chemistry plays a secondary role on radium and radon distributions as the ²²²Rn/²²⁶Ra activity ratio is correlated with redox-sensitive solutes such as dissolved oxygen and Mn concentrations, as well as overall dissolved solids content including major divalent cations and Ba. Since ²²⁴Ra/²²⁸Ra activity ratios in groundwater are close to 1, we suggest that mobilization of Ra and Rn is controlled by alpha recoil processes from parent nuclides on fracture surfaces, ruling out Ra sources from mineral dissolution or significant long-distance Ra transport. Alpha recoil is balanced by Ra adsorption that is influenced by redox conditions and/or ion concentrations, resulting in an approximately one order of magnitude decrease (~ 20,000 to ~ 2000) in the apparent Ra distribution coefficient between oxygen-saturated and anoxic conditions and also across the range of dissolved ion concentrations (up to ~ 7 mM). Thus, the U and Th content of rocks is the primary control on observed Ra and Rn activities in groundwater in fractured crystalline rocks, and in addition, linked dissolved solids concentrations and redox conditions impart a secondary control.     

Radium isotopic measurements in the search for uranium in palaeodrainage channels

Analyses have been made of many groundwater samples, some of which were collected from the vicinity of uranium deposits and others from unmineralized areas, for dissolved uranium and for the four naturally occurring isotopes of radium: ²²⁶Ra (²³⁸U decay series, y), ²²⁸Ra and ²²⁴Ra (²³²Th decay series, y and 3.8 d) and ²²³Ra (²³⁵U decay series, d). The radium isotopes ²²⁶Ra, ²²⁴Ra and ²²³Ra, are measured by alpha-spectrometry after extraction from a water sample soon after collection and ²²⁸Ra at a later time by determining the amount of ingrown ²¹²Po.     

Evaluation of the 210Po method at the Midwest uranium deposit,Northern Saskatchewan,Canada

Vertical profiles of ²¹⁰Po in soils near the Midwest uranium deposit and an associated surficial radioactive sandstone boulder train in northern Saskatchewan show a high ²¹⁰Po background in air-dried forest litter (24 pCi/g) and Ah horizon soil (11 pCi/g) relative to lower soil horizons (<1 pCi/g). These high levels mask the ²¹⁰Po signal from the radioactive boulders in the near-surface soil horizons. Only in the Bf and C horizons can the existence of the radioactive boulders be inferred from ²¹⁰Po determinations. For comparative purposes profiles for ²²⁶Ra, U, Ni, and other trace elements are also presented.Escape of most of the Rn from near surface soils into the atmosphere, homogenization and decay of Rn, and precipitation of decay products back onto surface soils satisfactorily explain the field observations discussed here.Compared to the highly anomalous ²²²Rn signal in soil gases over this boulder train the ²¹⁰Po contrast is very weak and is of little use for prospecting for this type of boulder train. The relatively high ²¹⁰Po background in surficial materials relative to lower soil horizons dictates that great care be taken with the ²¹⁰Po method; the deepest possible horizons should be sampled.     

The source of radium in anomalous accumulations near sandstone escarpments,Australia

The source of Ra has been determined in water samples from four areas in Australia where anomalously high surface concentrations of²²⁶Ra have accumulated from groundwaters. All four anomalies were located adjacent to sandstone formations, and the groundwaters, which were generally all acidic and low in dissolved salts, appeared to be meteoric water with short ground-residence times. Uranium,²²⁶Ra and²²⁸Ra concentrations of waters feeding the anomalous areas were comparable to those found in standing waters within the sandstones. The²²⁶Ra/²²⁸Ra isotopic ratios were distributed about a median of 1.1 which suggests that the waters are in contact with rocks with near-normal U/Th ratios and, hence, that the Ra in the anomalies was derived from within the sandstones.The presence of the short-lived Ra isotopes,²²³Ra and²²⁴Ra, in high concentrations in most spring waters feeding these anomalies suggests that Ra enters groundwaters by recoil following alpha decay of a precursor parent radionuclide within mineral grains. Thus, although three of the areas were considered prospective for U, the radioactive anomalies studied appear to be due to natural transfer of Ra from the sandstones to the surface environment. In no case were the anomalies related to nearby known or undiscovered U deposits. Accordingly, a geochemical procedure, which includes Ra isotopic measurements, is recommended for evaluating radioactive anomalies for U exploration. This procedure should enable selection of only those anomalies with the highest potential for further exploration by more expensive techniques.     

Factors controlling tungsten concentrations in ground water,Carson Desert,Nevada

An investigation of a childhood leukemia cluster by US Centers for Disease Control and Prevention revealed that residents of the Carson Desert, Nevada, are exposed to high levels of W and this prompted an investigation of W in aquifers used as drinking water sources. Tungsten concentrations in 100 ground water samples from all aquifers used as drinking water sources in the area ranged from 0.27 to 742 μg/l. Ground water in which W concentrations exceed 50 μg/l principally occurs SE of Fallon in a geothermal area. The principal sources of W in ground water are natural and include erosion of W-bearing mineral deposits in the Carson River watershed upstream of Fallon, and, possibly, upwelling geothermal waters. Ground water in the Fallon area is strongly reducing and reductive dissolution of Fe and Mn oxyhydroxides may be releasing W; however, direct evidence that the metal oxides contain W is not available.Although W and Cl concentrations in the Carson River, a lake, and water from many wells, appear to be controlled by evaporative concentration, evaporation alone cannot explain the elevated W concentrations found in water from some of the wells. Concentrations of W exceeding 50 μg/l are exclusively associated with $\mathrm{Na}''–''{\mathrm{HCO}}_3$ and Na–Cl water types and pH > 8.0; in these waters, geochemical modeling indicates that W exhibits <10% adsorption. Tungsten concentrations are strongly and positively correlated with As, B, F, and P, indicating either common sources or common processes controlling their concentrations. Geochemical modeling indicates W concentrations are consistent with pH-controlled adsorption of W.The geochemical model PHREEQC was used to calculate IAP values, which were compared with published Ksp values for primary W minerals. FeWO₄, MnWO₄, Na₂WO₄, and MgWO₄ were undersaturated and CaWO₄ and SrWO₄ were approaching saturation. These conclusions are tentative because of uncertainty in the thermodynamic data.The similar behavior of As and W observed in this study suggests ground water in areas where elevated As concentrations are present also may contain elevated W concentrations, particularly if there is a mineral or geothermal source of W and reducing conditions develop in the aquifer.     

An investigation about natural radioactivity,hydrochemistry, and metal pollution in groundwater from Calabrian selected areas,southern Italy

The increasing interest in radioactivity has brought about the need for an assessment of human exposure to radiation. It is, therefore, necessary to examine naturally occurring radioactivity in the environment, especially its occurrence in groundwater. The aim of this work was then to study the levels and behavior of the most significant natural radionuclides, also in order to improve the knowledge of the hydrochemical processes involved in the selected groundwater systems. Natural radioactivity in fifteen Calabrian groundwaters for human use was investigated through high-resolution gamma spectrometry (with a negative-biased Ortec HPGe detector) and liquid scintillation measurements. Particular attention was given on those radionuclides (³H, ²³⁸U, ²²⁶Ra, and ²²⁸Ra), which contribute in a significant way to the overall effective dose received by members of the public due to the intake of drinking water originating from groundwater systems. The activity concentration of ²³⁸U varied from 1 to 51 mBq/L, as a result of the geology of the investigated area and of the oxidizing conditions that favored U dissolution. ²²⁶Ra presented a broad range of activity concentrations (0.011–0.14 mBq/L), lower than uranium ones because radium occurs in groundwater under reducing conditions. Some heavy metals (Cd, Pb, Be, Hg, Ag, As, Tl, Sb, Se, and Ni) were also investigated through ICP-MS measurements and compared with the limits set by the Italian Legislation. Metals are released into the environment by both natural and anthropogenic sources; they leach into underground waters, moving along water pathways and eventually depositing in the aquifer.     

Geochemical evaluation of flowback brine from Marcellus gas wells in Pennsylvania,USA

Large quantities of highly saline brine flow from gas wells in the Marcellus Formation after hydraulic stimulation (“fracking”). This study assesses the composition of these flowback waters from the Marcellus shale in Pennsylvania, USA. Concentrations of most inorganic components of flowback water (Cl, Br, Na, K, Ca, Mg, Sr, Ba, Ra, Fe, Mn, total dissolved solids, and others) increase with time from a well after hydraulic stimulation. Based on results in several datasets reported here, the greatest concentration of Cl⁻ in flowback water is 151,000 mg/L. For total Ra (combined ²²⁶Ra and ²²⁸Ra) in flowback, the highest level reported is 6540 pCi/L. Flowback waters from hydraulic fracturing of Marcellus wells resemble brines produced from conventional gas wells that tap into other Paleozoic formations in the region. The Br/Cl ratio and other parameters indicate that both types of brine formed by the evaporation of seawater followed by dolomitization, sulfate reduction and subsurface mixing with seawater and/or freshwater. Trends and relationships in brine composition indicate that (1) increased salt concentration in flowback is not mainly caused by dissolution of salt or other minerals in rock units, (2) the flowback waters represent a mixture of injection waters with highly concentrated in situ brines similar to those in the other formations, and (3) these waters contain concentrations of Ra and Ba that are commonly hundreds of times the US drinking water standards.     

Determination of radioactivity levels in Akhisar,Gördes,Gölmarmara and Sindirgi regions,Western Turkey

In this study, radioactivity measurements in the environment of Akhisar, Gölmarmara, Gördes and Sindirgi regions in Western Turkey were investigated in order to evaluate the implications of any excess radioactivity in the environment of geological formation. The radioactivity concentrations of ⁴⁰K, ²³⁸U and ²³²Th radionuclides in the soil samples were measured by a NaI(Tl) gamma spectrometer system, and the radium activity concentrations in the water samples were also analyzed by an ZnS(Ag) alpha counter by the collector chamber method. The radioactivity of ⁴⁰K, ²³⁸U and ²³²Th in soils ranged 2.80–2,347.77, 9.90–256.19 and 9.66–106.53 Bq kg^?1, respectively. The activity of ²²⁶Ra in the water samples ranged from 0.03 Bq L^?1 (0.89pCi/L) to 0.80 Bq L^?1 (21.58pCi/L). In addition, the external terrestrial gamma dose rate in air (nGy h^?1), annual effective dose rate (mSv year^?1) and radium equivalent activity (Bq kg^?1) were calculated and compared with international standard values.     

Alpha-emitting isotopes and chromium in a coastal California aquifer

The unadjusted 72-h gross alpha activities in water from two wells completed in marine and alluvial deposits in a coastal southern California aquifer 40 km north of San Diego were 15 and 25 picoCuries per liter (pCi/L). Although activities were below the Maximum Contaminant Level (MCL) of 15 pCi/L, when adjusted for uranium activity; there is concern that new wells in the area may exceed MCLs, or that future regulations may limit water use from the wells. Coupled well-bore flow and depth-dependent water-quality data collected from the wells in 2011 (with analyses for isotopes within the uranium, actinium, and thorium decay-chains) show gross alpha activity in marine deposits is associated with decay of naturally-occurring ²³⁸U and its daughter ²³⁴U. Radon activities in marine deposits were as high as 2230 pCi/L. In contrast, gross alpha activities in overlying alluvium within the Piedra de Lumbre watershed, eroded from the nearby San Onofre Hills, were associated with decay of ²³²Th, including its daughter ²²⁴Ra. Radon activities in alluvium from Piedra de Lumbre of 450 pCi/L were lower than in marine deposits. Chromium VI concentrations in marine deposits were less than the California MCL of 10 μg/L (effective July 1, 2014) but δ⁵³Cr compositions were near zero and within reported ranges for anthropogenic chromium. Alluvial deposits from the nearby Las Flores watershed, which drains a larger area having diverse geology, has low alpha activities and chromium as a result of geologic and geochemical conditions and may be more promising for future water-supply development.     

Uranium series disequilibrium in a young surficial uranium deposit,northeastern Washington,U.S.A.

A recently discovered ore-grade accumulation of U in organic-rich sediments of late Quaternary age provides an opportunity for studying the early association of U, U-daughters, and organic matter in a natural setting. The U occurs in valley-fill sediments of peat, peaty clay, silt, and sand along the north fork of Flodelle Creek, Stevens County, Washington. Radiometric techniques (delayed neutron, high-resolution gamma-ray spectrometry, thin-source alpha spectrometry) were employed to determine the abundance and distribution of U-series nuclides, the extent of secular equilibrium within the U decay series, and the apparent U-series ages of U incorporation.Sixteen lithologically distinct intervals were sampled from a 292 cm core. Uranium contents range from 140 to 2790 ppm and are positively correlated with organic contents. Measured alpha activity ratios of ²³⁴U/²³⁸U (1.31–1.38) are very similar to those reported in coexisting waters, suggesting a rather constant isotopic composition of introduced U. Much lower Th contents of <10–40 ppm are controlled by the type and abundance of silicate detritus. The youth of the host sediments (<15 000 a) and the paucity of associated radioactivity suggested large excesses of U relative to radioactive daughters and such excesses were observed, particularly in the shallowest intervals. Apparent ages of U emplacement determined by the (alpha) activity ratio of ²³⁰Th daughter to ²³⁴U parent show a general increase with depth and fair agreement with estimated depositional ages. This observation suggests dominantly syndepositional or early post depositional emplacement of U followed by decay-generated buildup of ²³⁰Th daughter with time. However, interval by interval comparisons of the relative abundances of other daughters, particularly ²²⁶Ra and ²¹⁰Pb, indicate variability caused by processes other than closed-system growth and decay, probably because chemically diverse daughters that are decay-generated in situ have differing mobilities and because upwelling ground water continuously adds more U and minor amounts of daughters. If ²³⁰Th is considered the least susceptible to these modifications, the data suggest some addition of ²³⁴U in the deepest intervals and some loss of ²²⁶Ra and/or gain of ²²²Rn throughout the studied core.     

Natural radioactivity levels and evaluation of radiological hazards from Beni Haroun dam sediment samples,northeast Algeria

Levels of naturally occurring radioactivity in sediment samples of Beni Haroun dam have been investigated. The activity concentrations of ²³⁸U and ²³²Th decay chains and ⁴⁰K primordial radionuclide have been measured using high-resolution HPGe detector. Activity concentrations of ²²⁶Ra, ²³²Th, and ⁴⁰K radionuclides were found in the ranges 9–66, 14–37, and 177–288 Bq/kg with the mean values 24.67, 25.98, and 208.10 Bq/kg, respectively. Radiological hazard parameters were estimated based on the activity concentrations for ²²⁶Ra, ²³²Th, and ⁴⁰K to find out any radiation hazard associated with the sediments. Correlation studies between pairs of radionuclides were performed and discussed, and the obtained results are compared with international recommended values.     

US Geological Survey research on the environmental fate of uranium mining and milling wastes

Studies by the US Geological Survey (USGS) of uranium mill tailings (UMT) have focused on characterizing the forms in which radionuclides are retained and identifying factors influencing the release of radionuclides to air and water. Selective extraction studies and studies of radionuclide sorption by and leaching from components of UMT showed alkaline earth sulfate and hydrous ferric oxides to be important hosts of radium-226 (²²⁶Ra) in UMT. Extrapolating from studies of barite dissolution in anerobic lake sediments, the leaching of²²⁶Ra from UMT by sulfate-reducing bacteria was investigated; a marked increase in²²⁶Ra release to aqueous solution as compared to sterile controls was demonstrated. A similar action of iron(III)-reducing bacteria was later shown. Ion exchangers such as clay minerals can also promote the dissolution of host-phase minerals and thereby influence the fate of radionuclides such as²²⁶Ra. Radon release studies examined particle size and ore composition as variables. Aggregation of UMT particles was shown to mask the higher emanating fraction of finer particles. Studies of various ores and ore components showed that UMT cannot be assumed to have the same radon-release characteristics as their precursor ores, nor can²²⁶Ra retained by various substrates be assumed to emanate the same fraction of radon. Over the last decade, USGS research directed at offsite mobility of radionuclides from uranium mining and milling processes has focused on six areas: the Midnite Mine in Washington; Ralston Creek and Reservoir, Colorado; sites near Canon City, Colorado; the Monument Valley District of Arizona and Utah; the Cameron District of Arizona; and the Puerco River basin of Arizona and New Mexico.     

Factors controlling the groundwater transport of U, Th, Ra, and Rn

A model for the groundwater transport of naturally occurring U, Th, Ra, and Rn nuclides in the²³⁸U and²³²Th decay series is discussed. The model developed here takes into account transport by advection and the physico-chemical processes of weathering, decay, α-recoil, and sorption at the water-rock interface. It describes the evolution along a flowline of the activities of the²³⁸U and²³²Th decay series nuclides in groundwater. Simple sets of relationships governing the activities of the various species in solution are derived, and these can be used both to calculate effective retardation factors and to interpret groundwater data. For the activities of each nuclide, a general solution to the transport equation has been obtained, which shows that the activities reach a constant value after a distance ϰ_i, characteristic of each nuclide. Where ϰ_i is much longer than the aquifer length, (for²³⁸U,²³⁴U, and²³²Th), the activities grow linearly with distance. Where gKⁱ is short compared to the aquifer length, (for²³⁴Th,²³⁰Th,²²⁸Th,²²⁸Ra, and²²⁴Ra), the activities rapidly reach a constant or quasi-constant activity value. For²²⁶Ra and²²²Rn, the limiting activity is reached after 1 km. High δ²³⁴U values (proportional to the ratio^ɛ234Th/^W238U) can be obtained through high recoil fraction and/or low weathering rates. The activity ratios²³⁰Th/²³²Th,²²⁸Ra/²²⁶Ra and²²⁴Ra/²²⁶Ra have been considered in the cases where either weathering or recoil is the predominant process of input from the mineral grain. Typical values for weathering rates and recoil fractions for a sandy aquifer indicate that recoil is the dominant process for Th isotopic ratios in the water. Measured data for Ra isotope activity ratios indicate that recoil is the process generally controlling the Ra isotopic composition in water. Higher isotopic ratios can be explained by different desorption kinetics of Ra. However, the model does not provide an explanation for²²⁸Ra/²²⁶Ra and²²⁴Ra/²²⁶Ra activity ratios less than unity. From the model, the highest²²²Rn emanation equals 2ɛ. This is in agreement with the hypothesis that²²²Rn activity can be used as a first approximation for input by recoil (Krishnaswamiet al 1982). However, high²²²Rn emanation cannot be explained by production from the surface layer as formulated in the model. Other possibilities involve models including surface precipitation, where the surface layer is not in steady-state.     

Hydrologic controls on water chemistry and mercury biotransformation in a closed river system: The Carson River,Nevada

The Carson River flows in a closed basin system and the total flow of the river water decreases downstream due to both evaporation and consumptive uses. This river system is fed primarily by snow pack in the Sierra Nevada during the winter, which flows down gradient following melting in spring and summer. Water loss through evaporation in the Carson River results in a downstream buildup of conservative elements such as Cl⁻ and certain oxyanion forming elements including Se, Mo and W, which are known to interfere with the transformation of Hg within the S cycle. In addition to these naturally occurring hydrologic processes and the resulting affects on water chemistry, the Carson River Basin has been historically impacted by Au and Ag mining that used Hg amalgamation techniques. Contamination of Hg in the Carson River system is now well documented and published Hg concentrations in different environmental compartments are extremely high. In this study, hydrologically driven changes in water chemistry of the river system and the resulting effects on Hg cycling were examined. Results show that periods of low water flow correspond to high water pH (up to 8.3), relatively high concentrations of oxyanion forming elements (e.g., As, Se, Mo and W), and low Hg methylation potential in sediment. In contrast, periods of high flow bring about dilution, which results in lower pH (∼7), lower concentrations of oxyanion forming elements, but higher Hg methylation potential. Overall, changes in flow regimes likely affect rates of methyl-Hg (MeHg) production through a combination of factors such as high pH, which favors MeHg demethylation, and the occurrence of relatively high concentrations of Group VI oxyanions that could interfere with microbial SO₄ reduction and MeHg production.     

Occurrence and geochemistry of radium in water from principal drinking-water aquifer systems of the United States

A total of 1270 raw-water samples (before treatment) were collected from 15 principal and other major aquifer systems (PAs) used for drinking water in 45 states in all major physiographic provinces of the USA and analyzed for concentrations of the Ra isotopes ²²⁴Ra, ²²⁶Ra and ²²⁸Ra establishing the framework for evaluating Ra occurrence. The US Environmental Protection Agency Maximum Contaminant Level (MCL) of 0.185 Bq/L (5 pCi/L) for combined Ra (²²⁶Ra plus ²²⁸Ra) for drinking water was exceeded in 4.02% (39 of 971) of samples for which both ²²⁶Ra and ²²⁸Ra were determined, or in 3.15% (40 of 1266) of the samples in which at least one isotope concentration (²²⁶Ra or ²²⁸Ra) was determined. The maximum concentration of combined Ra was 0.755 Bq/L (20.4 pCi/L) in water from the North Atlantic Coastal Plain quartzose sand aquifer system. All the exceedences of the MCL for combined Ra occurred in water samples from the following 7 PAs (in order of decreasing relative frequency of occurrence): the Midcontinent and Ozark Plateau Cambro-Ordovician dolomites and sandstones, the North Atlantic Coastal Plain, the Floridan, the crystalline rocks (granitic, metamorphic) of New England, the Mesozoic basins of the Appalachian Piedmont, the Gulf Coastal Plain, and the glacial sands and gravels (highest concentrations in New England).     

Naturally occurring radionuclides and their geochemical interactions at a geothermal site in the North German Basin

The activities of the most common, naturally occurring radionuclides ²³⁸U, ²²⁶Ra, ²¹⁰Pb, ²²⁸Ra, ²²⁸Th, and ⁴⁰K were measured by gamma-ray spectrometry in samples from reservoir rocks, geothermal fluids, and mineral precipitates at the geothermal research site Groß Schönebeck (North German Basin). Results demonstrated that the specific activity of the reservoir rock is within the range of the mean concentration in the upper earth crust of <800 Bq/kg for ⁴⁰K and <60 Bq/kg for radionuclides of the ²³⁸U and ²³²Th series, respectively. The geothermal fluid showed elevated activity concentrations (up to 100 Bq/l) for ²²⁶Ra, ²¹⁰Pb, and ²²⁸Ra, as compared to concentrations found in natural groundwater. Their concentration in filter residues even increased up to 100 Bq/g. These residues contain predominantly two different mineral phases: a Sr-rich barite (Sr, BaSO₄) and laurionite (PbOHCl), which both precipitate upon cooling from the geothermal fluid. Thereby they presumably enrich the radionuclides of Ra (by substitution of Ba) and Pb. Analysis of these precipitates further showed an increased ²²⁶Ra/²²⁸Ra ratio from around 1–1.7 during the initial months of fluid production indicating a change in fluid composition over time which can be explained by different contributions of stimulated reservoir rock areas to the overall produced fluid.     

Natural or fertilizer-derived uranium in irrigation drainage: a case study in southeastern Colorado,U.S.A.

Drainage from heavily cultivated soils may be contaminated with U that is leached from the soil or added as a trace constituent of PO₄-based commercial fertilizer. The effect of decades-long application of U-rich fertilizer on the U concentration of irrigation drainage was investigated in a small (14.2 km²) drainage basin in southeastern Colorado. The basin was chosen because previous reports indicated locally anomalous concentrations of dissolved NO₃ (6–36 mg 1⁻¹) and dissolved U (61 pg 1⁻¹) at the mouth of the only stream. Results of this study indicated minimal impact of fertilizer-U compared to natural U leached from the local soils. Detailed sampling of the stream along a 6 mile (9.7 km) reach through heavily cultivated lands indicated marked decoupling of the buildup of dissolved NO₃ and U. Dissolved U increased markedly in the upstream half of the reach and correlated positively with increases in Na, Mg, SO₄, B and Li derived from leaching of surrounding shaley soils. In contrast, major increases in dissolved NO₃ occurred farther downstream where stream water was heavily impacted by ground water return from extensively fertilized fields. Nitrogen isotopic measurements confirmed that dissolved NO₃ originated from fertilizer and soil organic N (crop waste). Uranium isotopic measurements of variably uraniferous waters showed little evidence of contamination with fertilizer-derived U of isotopically distinct²³⁴U/²³⁸U alpha activity ratio (A.R. = 1.0). Leaching experiments using local alkaline soil, irrigation water and U-rich fertilizer confirmed the ready leachability of soil-bound U and the comparative immobility of U added with liquid fertilizer. Relatively insoluble precipitates containing CaPU were formed by mixing liquid fertilizer with water containing abundant dissolved Ca. In the local soils soluble Ca is provided by dissolution of abundant gypsum. Similar studies are needed elsewhere because the mobility of fertilizer-derived U is dependent on fertilizer type, porewater chemistry and soil properties (pH, moisture, mineralogy, texture).