Evaluation of radioactive anomalies using radium isotopes in ground waters

An empirical scheme based on the concentrations of uranium and the three alpha-emitting radium isotopes ²²⁶Ra, ²²⁴Ra and ²²³Ra is proposed for rating the significance of ground waters with respect to uranium exploration. The scheme has been developed from the results for over 200 water samples from the vicinity of known uranium deposits and radium anomalies in areas of Australia with climates varying from arid to tropical. The scheme uses relative levels of the four factors to rate the potential of a sample as good, possible or poor. An example of the use of the system in ground-water exploration in the Frome Embayment, South Australia, is presented to illustrate the value of the scheme in rejecting falsely anomalous samples with high uranium concentrations whilst detecting nearby uranium mineralization from drill holes not intersecting mineralization.     

Radium isotopes in saline seepages,south-western Yilgarn,Western Australia

Water samples from saline seepages in the south-western Yilgarn Block of Western Australia contain high activities of the four naturally-occurring radium isotopes. Activities of up to 310 $\text{pCi}\text{l}$ for ²²⁶Ra and 1720 $\text{pCi}\text{l}$ for ²²⁸Ra were measured and the ${}^{228}\text{Ra}{}^{226}\text{Ra}$ ratio averaged 6.1. Activities of the two short-lived radium isotopes were also high. ²²³Ra activities of up to 94 $\text{pCi}\text{l}$ were found with an average ${}^{226}\text{Ra}{}^{223}\text{Ra}$ ratio of 3.3, considerably lower than the natural abundance ratio of 21.4. Activities of up to 23 $\text{pCi}\text{l}$²²⁷Ac, the long-lived ($\text{t}{}_{\mathrm{<mtext>1</mtext><mtext>2</mtext>}}\text{= 22 years}$) grandparent of ²²³Ra, were also measured. The analysis of surface granite samples, the probable source rocks of the radium, gave $\text{Th}\text{U}$ activity ratios of around 1.5. The higher ${}^{228}\text{Ra}{}^{226}\text{Ra}$ ratios of the waters were attributed to readily leached ²²⁸Ra in the weathered granites as a result of thorium remaining after weathering. Leach experiments on U-Th ore by NaCl solutions showed that all four radium isotopes were equally leached. Sulphate anions reduced the ²²⁶Ra and ²²⁸Ra leaching to a greater extent than for ²²³Ra and ²²⁴Ra, suggesting that the latter isotopes were being supported in solution by parent isotopes. In particular this suggested ²²⁷Ac was leached into the sulphate solution but this does not fully account for the amount of ²²⁷Ac seen in the seepage waters.     

Evaluation of lead isotopic methods for uranium exploration, Koongarra Area, Northern Territory, Australia

Analysis of radioactive (²¹⁰Pb) and stable lead isotopes in near-surface samples has been tested as a method of uranium exploration in the Pine Creek Geosyncline, Northern Territory, Australia. The lead isotopes were extracted from the samples by a mild leaching agent and were measured by alpha spectrometry for ²¹⁰Pb and by mass spectrometry for stable lead isotopes. The results are compared with those obtained by conventional methods utilizing measurements of radioactivity and radon (Track Etch) in situ and ²²⁶Ra, ²²⁸Ra and U contents of soils. The major problems addressed were whether the lead isotopic methods are more sensitive than the conventional methods and whether they can discriminate “real” anomalies from the common barren anomalies found in black soils and swamps which contain radium in excess of the uranium present.Four test areas, representing a range of exploration problems, were chosen in the vicinity of the Koongarra uranium deposits and 25 samples from each area were analyzed. Most samples have more ²²⁶Ra than uranium. Radium analyses of several water samples show the source of this radium to be non-uraniferous rocks within the Kombolgie sandstone. The results for soil ²²⁶Ra, radon, scintillometry and ²¹⁹Pb were generally closely correlated, and as a result, the ²¹⁰Pb method was not considered to have any advantages over the conventional methods.At the Koongarra X prospect, which has a weak surface expression, the ratio gave the strongest indication of the underlying uranium mineralization with an anomaly to background ratio of 12.5. However, this ratio is correlated with uranium content and does not offer any particular advantages over uranium analyses alone. More subtle indications of uranium mineralization were found by relating the radiogenic lead (²⁰⁶Pb) and the thorium-derived lead (²⁰⁸Pb) to the common lead content (²⁰⁴Pb). A plot of versus (horizontal axis) is linear for country rock samples, irrespective of the amount of more recently introduced ²²⁶Ra. Samples above uranium mineralization lie off this trend, along a line of near-zero slope. By the use of this plot, indications were found of the Koongarra No. 2 orebody, which is concealed by about 40 m of barren overburden; none of the other techniques detected this mineralization.     

Ra and Th adsorption coefficients in lakes—Lake Kinneret (Sea of Galilee) “natural experiment”

The adsorption rate constants of Ra and Th were estimated from empirical data from a freshwater lake and its feeding saline springs. We utilized the unique setting of Lake Kinneret (Sea of Galilee, northern Israel) in which most of the Ra and Th nuclides are introduced into the lake by saline springs with high ²²⁶Ra activities and a high ²²⁴Ra/²²⁸Ra ratio of 1.5. The mixing of the Ra enriched saline waters and freshwater in the lake causes the ²²⁴Ra/²²⁸Ra ratio to drop down to 0.1 in the Kinneret due to preferential adsorption of ²²⁸Th. These conditions constitute a “natural experiment” for estimating adsorption rates. We developed a simple mass-balance model for the radionuclides in Lake Kinneret that accurately predicted the Ra isotope ratios and the ²²⁶Ra activity in the lake. The model is comprised of simultaneous equations; one for each radionuclide. The equations have one input term: supply of radionuclides from the saline springs; and three output terms: adsorption on particles in the lake, radioactive decay and outflow from the lake. The redundancy in the analytical solutions to the mass balance equations for the relevant nuclides constrained the values of Ra and Th adsorption rate constants to a very narrow range. Our results indicate that the adsorption rate constant for Ra is between 0.005 d⁻¹ and 0.02 d⁻¹. The rate constant for Th is between 0.5 d⁻¹ and 1 d⁻¹, about fifty to a hundred times higher. The estimated desorption rate coefficient for Ra is about 50-100 times larger than its adsorption rate constant. The mass-balance equations show that the residence times of all Ra isotopes (²²⁶Ra, ²²⁸Ra,²²³Ra, ²²⁴Ra) and of ²²⁸Th in the lake are about 95, 92, 14, 6 and 1 d, respectively. These residence times are much shorter than the residence time of water in the lake (about 5.5 y). The steady state activity ratios in Lake Kinneret depend mainly on the adsorption rate constants, decay constants, the outflow rate from the lake and the activity ratios in the saline springs. The activity ratios are independent of the saline springs flow rate.     

Application of radium isotopes to determine crustal residence times of hydrothermal fluids from two sites on the Reykjanes Peninsula, Iceland

Radium isotopes were used to determine the crustal residence times of hydrothermal fluids from two geothermal wells (Svartsengi and Reykjanes) from the Reykjanes Peninsula, Iceland. The availability of rock samples from the subsurface (to depths of 2400 m) allowed direct comparison of the radium isotopic characteristics of the fluids with those of the rocks within the high temperature and pressure reaction zone. The ²²⁶Ra activity of the Svartsengi fluid was ∼one-fourth of the Reykjanes fluid and the ²²⁸Ra/²²⁶Ra ratio of the Svartsengi fluid was ∼twice that of Reykjanes. The fluid isotopic characteristics were relatively stable for both sites over the 6 years (2000-2006) of the study. It was determined, using a model that predicts the evolution of the fluid ²²⁸Ra/²²⁶Ra ratio with time, that both sites had fluid residence times, from the onset of high temperature water-rock reaction, of less than 5 years. Measurement of the short-lived ²²⁴Ra and ²²³Ra allowed estimation of the recoil input parameter used in the model. The derived timescale is consistent with results from similar studies of fluids from submarine systems, and has implications for the use of terrestrial systems in Iceland as an exploited energy resource.     

Application of226Ra,228Ra,223Ra, and224Ra in coastal waters to assessing coastal mixing rates and groundwater discharge to oceans

The fate of dissolved material delivered to the coastal ocean depends on its reactivity and the rate at which it is mixed offshore. To measure the rate of exchange of coastal waters, we employ two short-lived radium isotopes,²²³Ra and²²⁴Ra. Along the coast of South Carolina, shore-perpendicular profiles of²²³Ra and²²⁴Ra in surface waters show consistent gradients which may be modeled to yield eddy diffusion coefficients of 350–540 m²s⁻¹. Coupling the exchange rate with offshore concentration gradients yields estimates of offshore fluxes of dissolved materials. For systems in steady state, the offshore fluxes must be balanced by new inputs from rivers, groundwater, sewers or other sources. Two tracers that show promise in evaluating groundwater input are barium and²²⁶Ra. These tracers have high relative concentrations in the fluids and low-reactivity in the coastal ocean. Applying the eddy diffusion coefficients to the offshore gradient of²²⁶Ra concentration provides an estimate of the offshore flux of²²⁶Ra. Measuring the concentrations of²²⁶Ra in subsurface fluids provides an estimate of the fluid flux necessary to provide the²²⁶Ra. These estimates indicate that the volume of groundwater required to support these fluxes is of the order of 40% of the surface water flow.     

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.     

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.     

An improved method for Ra isotope (226Ra, 228Ra, 224Ra) measurements by gamma spectrometry in natural waters: application to CO2-rich thermal waters from the French Massif Central

An improved method was developed to measure ²²⁶Ra, ²²⁸Ra and ²²⁴Ra in freshwaters by gamma spectrometry. Radium was selectively extracted from acidified samples using specific filters (3M EMPORE™ Radium Rad disks). The latter was subsequently analysed by gamma spectrometry. Simultaneous and direct determination of the activities of the three isotopes was performed by comparison of gamma rays of the Radium Rad disks with those of a calibrated standard disk. This efficient and reliable method allowed a reduction of sample processing to a few hours.This technique was applied to analyse the Ra isotope compositions of several CO₂-rich hydrothermal springs of the western border of the Limagne graben (French Massif Central). The studied springs emerge from a succession of granitic outcrops lined up along a major fault. Their chemical compositions evolve from calcic and magnesian chloro-bicarbonated to sodic bicarbonated. All the springs display high Ra activities, probably linked to high CO₂ content and/or high cation content of these waters, with various Ra isotope ratios. ²²⁶Ra activity ranges from 588 to 2287 mBq/l and ²²⁸Ra activity from 260 to 1590 mBq/l, whereas ²²⁴Ra displays an activity between 245 and 1808 mBq/l. Four of the six analysed springs have (²²⁸Ra/²²⁶Ra) activity ratios lower than 0.7, thus, significantly lower than the ratio expected from an interaction with a calc-alkaline granitoid (typically having (²³²Th/²³⁸U) activity ratio between 1 and 2). Low (²²⁸Ra/²²⁶Ra) ratio (0.27) of the northern water (Montpensier) suggests the existence in this area of a zone of U concentration, possibly resulting from U mobilization and accumulation induced by previous hydrothermal events. The (²²⁴Ra/²²⁸Ra) ratios display smaller variations. They suggest short transit times from the zone of Ra leaching to the surface (a few days) or a very shallow addition of ²²⁴Ra (e.g., from a localised zone where ²²⁸Th could be preferentially adsorbed on the mineral surfaces). In some cases, these ratios might be used to infer differences in transit times of waters between neighboring springs.     

Radium-based pore water fluxes of silica, alkalinity, manganese, DOC, and uranium: A decade of studies in the German Wadden Sea

A decade of studies of metal and nutrient inputs to the back-barrier area of Spiekeroog Island, NW German Wadden Sea, have concluded that pore water discharge provides a significant source of the enrichments of many components measured in the tidal channels during low tide. In this paper we add studies of radium isotopes to help quantify fluxes into and out of this system. Activities of radium isotopes in surface water from tidal channels in the back-barrier area exhibit pronounced changes in concert with the tide, with highest activities occurring near low tide. Other dissolved components: silica, total alkalinity (TA), manganese, and dissolved organic carbon (DOC) exhibit similar changes, with patterns matching the Ra isotopes. Uranium follows a reverse pattern with highest concentrations at high tide. Here we use radium isotope measurements in water column and pore water samples to estimate the fluxes of pore waters that enter the tidal channels during low tide. Using a flushing time of 4 days and the average activities of ²²⁴Ra, ²²³Ra, and ²²⁸Ra measured in the back-barrier surface and pore waters, we construct a balance of these isotopes, which is sustained by a deep pore water flux of (2-4) × 10⁸ L per tidal cycle. This flux transports Ra and the other enriched components to the tidal channels and causes the observed low tide enrichments. An independent estimate of pore water recharge is based on the depletion of U in the tidal channels. The U-based recharge is about two times greater than the Ra-based discharge; however, other sinks of U could reduce the recharge estimate. The pore waters have wide ranges of enrichment in silica, alkalinity, manganese, DOC, and depletion of U with depth. We estimate concentrations of these components in pore water from the depth expected to contribute the majority of the pore water flux, 3.5 m, to determine fluxes of these components to the tidal channels. Samples from this depth have minimum concentrations of silica, alkalinity, manganese, and DOC. We also estimate the exports of these components (and import of U) due to mixing based on average measured concentrations in the tidal creeks and the 4-day flushing time. A comparison of these estimates reveals that the exports (negative in the case of U) equal or exceed the pore water fluxes. By using values slightly higher than the minimum concentrations at 3.5 m to calculate inputs, the two estimates could be forced to match. We conclude that pore water drainage is the major factor regulating fluxes of Ra isotopes, silica, alkalinity, manganese, DOC, and uranium in this system.     

Radium Sampling Methods and Residence Times in St. Andrew Bay,Florida

Activity ratios (AR) of radium isotopes have been used with success to constrain estimates of water ages and to approximate residence times in coastal waters. We compared two common radium sampling methods (grab sampling and stationary moorings) to estimate water ages and the residence time of St. Andrew Bay waters in northwest Florida, USA. Both sampling methods utilize manganese dioxide fibers (“Mn fibers”) to adsorb dissolved radium from the water column. Grab samples capture radium activities at a discrete time while moorings integrate radium activities over longer deployments. The two methods yielded similar results in this study and thus both approaches are useful for water age comparisons and residence time approximations. However, since radium often varies as a function of tidal stage, deploying moorings over a complete tidal cycle is the preferred approach. An estimated residence time for North Bay and West Bay of 8–11 days was approximated using ARs for both ex²²⁴Ra/²²³Ra and ex²²⁴Ra/²²⁸Ra. Some complications were introduced as St. Andrew Bay is a tidally dominated, rather than a river-dominated bay system where this method has previously been applied. The largest freshwater source to this bay system is from a man-made reservoir, with an average freshwater flow of only 20 m³ s^?1. The activity concentrations and ARs measured by both sampling methods suggest that while the reservoir is the prominent radium source, it is not the only radium source. Nonetheless, a tidal mixing model applied to the western half of the system yielded an approximate flushing time of 10–12 days, similar to that derived from our radium-based water age approach.     

厦门火烧屿裸露岩石的铀放射系不平衡

用HPGeγ谱方法测定了厦门火烧屿裸露岩石天然放射性核素^40K、^228Ra、^228Th、^238U、^226Ra和^210Pb含量，对其铀系不平衡关系进行了讨论，发现钍系核素^228Ra和^228Th基本上是平衡的，而大部分样品^226Ra相对于^228U、^210Pb相对于^226Ra亏损。由此推论，水体作用下岸边岩石中^226Ra直接进入水体，可以是海水中^226Ra的一个来源；岸边岩石中^222Rn逸出后，衰变^210Pb再进入水体，可以是海水中^210Pb的一个来源。     

Development of a reactive zone technology for simultaneous in situ immobilisation of radium and uranium

Simultaneous in situ immobilisation of uranium (U) and radium (²²⁶Ra) by injectible amounts of grey cast iron (gcFe), nano-scale iron (naFe) and a gcFe/MnO₂ mixture (1:1) was studied in batch and column tests. Both 0.5 g/L naFe and gcFe are effective in ²²⁶Ra and U removal from mine water, whereas MnO₂ addition clearly increased the efficiency of gcFe for ²²⁶Ra and U immobilisation. In a column test with 0.6 wt% gcFe/MnO₂ mixture (1:1), neither ²²⁶Ra nor U was detected in the effluent after replacement of 45 pore volumes. A sequential extraction under flow condition revealed ²²⁶Ra to be mostly occluded in manganese oxides. Uranium was mostly sorbed onto poorly crystalline iron hydroxides, but a significant part was found to be occluded in manganese oxides also. The results of this study suggest that MnO₂ promotes iron hydroxide formation under slightly reducing environmental conditions resulting in an increased pollutant retention capacity.     

Variations of Hydrodynamics and Submarine Groundwater Discharge in the Yellow River Estuary Under the Influence of the Water-Sediment Regulation Scheme

The “Water-Sediment Regulation Scheme” (WSRS) is critically important to the hydrologic evaluation of the Yellow River estuary since a huge pulse of water and sediment are delivered into the sea during a short period. We used the natural geochemical tracers radium (²²³Ra, ²²⁴Ra, ²²⁶Ra) and radon (²²²Rn) isotopes as well as other hydrological parameters to investigate the mixing variations and submarine groundwater discharge (SGD) in the Yellow River estuary under the influence of the 2013 WSRS. Dramatically elevated radium and radon isotopic activities were observed during this WSRS compared with activities measured during a non-WSRS period. Radium “water ages” indicated that the offshore transport rate nearly tripled when the river discharge increased from 400 to 3400 m³/s. We calculated the SGD flux in the Yellow River estuary based on a radium mass balance model as well as radium and radon time-series models. The SGD flux was estimated at 0.02~0.20 m/day during a non-WSRS period and 0.67~1.22 m/day during the 2013 WSRS period. The results also indicate that large river discharge tends to lead more intense SGD along the river channel direction with a large amount of fresh SGD.     

The measurement of Ra/Ra activity ratios in ground water as a uranium exploration technique

Measurements were made of the ²²⁶Ra/²²³Ra activity ratio in ground waters obtained from drill holes in the vicinity of uranium mineralization in northern Saskatchewan where certain hydrologic parameters, specifically ground-water velocity and direction, had been determined. The results show that it is possible to approximate the distance from a ground-water sampling point to the area of mineralization owing to differences in the half lives of the two radium nuclides.The theoretical basis for the determination of the distances is explained.     

用镭同位素评价海水滞留时间及海底地下水排泄

海底地下水排泄(submarine groundwater discharge, SGD)难以直接测量, 镭同位素和氡-222等天然示踪剂使得间接评价SGD通量成为可能.为了评价五缘湾的水体滞留时间和SGD通量, 实测了湾内海水、湾外海水和地下水中224Ra和226Ra的活度, 利用224Ra和226Ra半衰期的差异, 采用224Ra与226Ra的活度比值计算湾内水团的年龄和平均滞留时间, 利用224Ra和226Ra的质量平衡模型计算SGD通量.五缘湾13个站位的水团年龄在0.6~2.4 d之间, 湾顶水团年龄相对较大, 平均海水滞留时间1.4 d.地下水输入五缘湾的224Ra和226Ra通量分别为5.17×106 Bq/d和5.28×106 Bq/d, 将该通量用地下水端元的活度转换成为SGD通量分别是0.21 m3/m2/d(224Ra平衡模型)和0.23 m3/m2/d(226Ra平衡模型), 两种模型的结果较接近, 其平均值0.22 m3/m2/d可作为五缘湾的海底地下水排泄通量.      

Radium geochemistry of ground waters in Paleozoic carbonate aquifers,midcontinent, USA

The purpose of this study was to elucidate the processes controlling the distribution and behavior of the longer-lived Ra isotopes in continuous Paleozoic carbonate aquifers of parts of Missouri, Kansas, and Oklahoma. Activities of (²²⁸Ra) and (²²⁶Ra) were analyzed in fresh and saline ground waters, brines, and rocks. The fluids have a wide salinity range (200–250,000 mg l⁻¹ total dissolved solids). The (²²⁶Ra) activity ranges from 0.66–7660 dpm kg⁻¹ and correlates with salinity and other alkaline earth element (Ca, Sr, and Ba) concentrations. The range of (²²⁸Ra:²²⁶Ra) ratios in the fluids (0.06–1.48) is similar to that in the aquifer rocks (0.21–1.53). The relatively low mean fluid (²²⁸Ra:²²⁶Ra) ratio (0.30) reflects the low Th:U ratio of the predominant carbonate aquifer rock. Radium occurs mostly (≥77%) as Ra²⁺ species in the fluids. Salinity-dependent sorption–desorption processes (with log K values from 10⁰–10⁴ and negatively correlated with salinity), involving Th-enriched surface coatings on aquifer flow channels, can explain the rapid solid–fluid transfer of Ra isotopes in the system and the correlation of Ra with salinity.     

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.