Ra-226 and Rn-222 in saline water compartments of the Aral Sea region

The Aral Sea has been shrinking since 1963 due to extensive irrigation and the corresponding decline in the river water inflow. Understanding of the current hydrological situation demands an improved understanding of the surface water/groundwater dynamics in the region. ²²²Rn and ²²⁶Ra measurements can be used to trace groundwater discharge into surface waters. Data of these radiometric parameters were not previously available for the study region. We determined ²²²Rn activities after liquid phase extraction using Liquid Scintillation Counting (LSC) with peak-length discrimination and analyzed ²²⁶Ra concentrations in different water compartments of the Amu Darya Delta (surface waters, unconfined groundwater, artesian water, and water profiles from the closed Large Aral Sea (western basin).The water samples comprise a salinity range between 1 and 263 g/l. The seasonal dynamics of solid/water interaction under an arid climate regime force the hydrochemical evolution of the unconfined groundwater in the Amu Darya Delta to high-salinity Na(Mg)Cl(SO₄) water types. The dissolved radium concentrations in the waters were mostly very low due to mineral over-saturation, extensive co-precipitation of radium and adsorption of radium on coexisting solid substrates.The analysis of very low ²²⁶Ra concentrations (<10 ppq) at remote study sites is a challenge. We used the water samples to test and improve different analytical methods. In particular, we modified a procedure developed for the α-spectrometric determination of ²²⁶Ra after solid phase extraction of radium using 3M Empore™ High Performance Extraction Disks (Purkl, 2002) for the analysis of the radionuclide using an ICP sector field mass spectrometer. The ²²⁶Ra concentration of 17 unconfined groundwater samples ranged between 0.2 and 5 ppq, and that of 28 artesian waters between <0.2 and 13 ppq. The ICP-MS results conformed satisfactorily to analytical results based on γ-measurements of the ²²²Rn ingrowth after purging and trapping on super-cooled charcoal. The ²²⁶Ra concentrations were positively correlated with the salinity and the dissolved NaCl concentrations. The occurrence of unusually high ²²⁶Ra activities is explained by radium release from adsorption sites with increasing salinity. The inferred spatial variability of ²²²Rn in the Aral Sea and of ²²²Rn and ²²⁶Ra in the groundwater of the Amu Darya Delta is discussed in the context of our own previous hydrochemical studies in the study sites. Relatively low ²²²Rn activities in the unconfined GW (1–9.5 Bq/l) indicate the alluvial sediments hosting the GW to be a low-²³⁸U(²²⁶Ra) substrate. Positive correlations between U and ²²⁶Ra, and U and ²²²Rn are likely related to locally deposited Fe(Mn)OOH precipitates. The ²²²Rn activity of the GW, however, distinctly exceeds the ²²²Rn concentration in the Aral Sea (10 mBq/l), in principle, making ²²²Rn a sensitive tracer for the inflow of GW. The high water volume of the Large Aral Sea and wind induced mixing of its water body, however, hamper the detection of local groundwater inflow.     

Relations of hydrogeologic factors, groundwater reduction-oxidation conditions, and temporal and spatial distributions of nitrate, Central-Eastside San Joaquin Valley, California, USA

In a 2,700-km² area in the eastern San Joaquin Valley, California (USA), data from multiple sources were used to determine interrelations among hydrogeologic factors, reduction-oxidation (redox) conditions, and temporal and spatial distributions of nitrate (NO₃), a widely detected groundwater contaminant. Groundwater is predominantly modern, or mixtures of modern water, with detectable NO₃ and oxic redox conditions, but some zones have anoxic or mixed redox conditions. Anoxic conditions were associated with long residence times that occurred near the valley trough and in areas of historical groundwater discharge with shallow depth to water. Anoxic conditions also were associated with interactions of shallow, modern groundwater with soils. NO₃ concentrations were significantly lower in anoxic than oxic or mixed redox groundwater, primarily because residence times of anoxic waters exceed the duration of increased pumping and fertilizer use associated with modern agriculture. Effects of redox reactions on NO₃ concentrations were relatively minor. Dissolved N₂ gas data indicated that denitrification has eliminated >5 mg/L NO₃–N in about 10% of 39 wells. Increasing NO₃ concentrations over time were slightly less prevalent in anoxic than oxic or mixed redox groundwater. Spatial and temporal trends of NO₃ are primarily controlled by water and NO₃ fluxes of modern land use.     

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.     

Dependence of radon exhalation on grain size of sedimentary waste

Tailings resulted from sulphuric acid leaching process of uranium from sedimentary rocks contain high concentrations of ²²⁶Ra and its daughters, the most important of which is ²²²Rn. Movement of radon gas out of the tailings is strongly influenced by the physicochemical characteristics of these tailings especially their radium content and the grain size. So, the tailing samples were size fractionated into four sizes (>?250, 250–125, 125–74 and <?74 µm). The natural radioactivity was investigated using hyper-pure germanium detector and solid-state nuclear track detectors (CR-39) for bulk size and after size fractionation. The activity concentrations of different radionuclides in size-fractionated tailing samples have been shown to be strongly dependent on the size of the particles. In the range of >?250 and <?74 µm, the activity concentrations of ²³⁰Th, ²²⁶Ra, ²¹⁴Pb, ²¹⁴Bi, ²¹⁰Pb, ²³²Th and ⁴⁰K increased throughout with decreasing particle size, while that of ²³⁸U, ²³⁴U and ²³⁵U have an opposite effect. The results revealed an inverse relationship between the radon exhalation rate and size fractionation. Also, the results showed a good correlation between radium activity concentration and radon mass exhalation rate.     

Natural Radon and Radium Isotopes for Assessing Groundwater Discharge into Little Lagoon,AL: Implications for Harmful Algal Blooms

Naturally occurring isotopes of radon (²²²Rn) and radium isotopes (^{223,224,226,228}Ra) were used as tracers to assess submarine groundwater discharge (SGD) into Little Lagoon, AL (USA), a site of recurring harmful algal blooms (HABs). The radium isotopic data suggests that there are two groundwater sources of these tracers to the lagoon, a shallow (A1) and deeper (A2) aquifer. We estimated the fraction of each source via a three-end-member mixing model consisting of Gulf of Mexico seawater, shallow and deep groundwater. The estimated lagoonwide SGD rates based on a radium mass balance and the mixing model were 1.22?±?0.53 and 1.59?±?0.20 m³ s^-1 for the shallow and deep groundwater discharges, respectively. To investigate temporal variations in SGD, we performed several radon surveys from 2010 through 2012, a period of generally declining groundwater levels due to a drought in the southeastern USA. The total SGD rates based on a radon mass balance approach were found to vary from 0.60 to 2.87 m³ s^-1. We observed well-defined relationships between nutrients and chlorophyll-a in lagoon waters during a period when there was an intense diatom bloom in April 2010 and when no bloom existed in March 2011. A good correlation was also found between radium (groundwater-derived) and nutrients during the April 2010 period, while there was no clear relationship between the same parameters in March 2011. Based on multivariate analysis of chemical and environmental factors, we suggest that nutrient-rich inputs during high SGD may be a significant driver of algal blooms, but during low SGD periods, multiple drivers are responsible for the occurrence of algal blooms.     

Geochemistry of granites and metasediments of the urban area of Vila Real (northern Portugal) and correlative radon risk

Radon concentration was evaluated in dwellings of the urban area of Vila Real (Northern Portugal). The area is mainly composed of Hercynian granites and Cambrian metasediments, and CR-39 passive detectors (n = 112) were used for the purpose. The results obtained in winter conditions suggest that the most productive geological unit is the Hercynian granite G1 (geometric mean of 364 Bq/m³), while Cambrian metasediments of the Douro Group show the lowest average indoor radon concentration (236 Bq/m³). The geological, geochemical and radiological data obtained suggest that the most effective control on the radon concentrations of the area is related with the uranium content of the rocks; indeed, the highest contents were observed in granite G1 (21 ppm) and the lowest in the metasediments (3 ppm). This is also confirmed by the results obtained for groundwater, where granites present the highest concentrations of dissolved radon (up to 938 Bq/l), uranium (5–18 ppb) and gross α activities (0.47–0.92 Bq/l). No important radiometric anomalies were found in relation with geological structures such as faults, veins and contacts, but a moderate increase of the uranium content can occur locally in such structures. Petrographic observations and SEM studies show that uranium is mainly contained within the rock in heavy accessory minerals (apatite, zircon, monazite, xenotime), which reduces radon emanation. Notwithstanding, due to the high U contents granites show a significant potential to induce indoor radon concentrations in dwellings in excess of the recommended value of 400 Bq/m³. Overall, we can conclude that the region of Vila Real presents a moderate to high radon risk in dwellings and groundwater.     

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.     

Radon-222 in medicinal groundwaters of Szczawno Zdrój (Sudety Mountains, SW Poland)

 Radon is a significant component of the groundwaters that discharge in the springs of Szczawno Zdrój and are recognized as medicinal. However, among the five exploited springs adjoining each other, it is only in Marta Spring that radon occurs in large concentrations (up to 325.6 Bq/dm³). Therefore, the authors have made an attempt to describe and clarify this fact. They found out from their own research and archival data that ²²²Rn dissolves in the waters of Marta Spring after acidulous waters of deep circulation have mixed with poorly mineralized shallow waters in their outflow zone. The genesis of the gas is determined by the content of its parent nuclide, ²²⁶Ra, in the sandstones in the vicinity of the intake. The volume of the rocks providing radon to the waters of this intake has been estimated at several hundred cubic metres. No seasonal fluctuations in radon concentration have been observed and ²²²Rn concentration changes do not seem to be influenced by changes in the concentration of other chemical components of the waters or by the discharge of the intake. The process of dissolving ²²²Rn in the medicinal groundwaters of Marta Spring is the last, the shortest, and the most local of the processes that form the chemical composition and the physical properties of these waters. Received: 7 January 2000 · Accepted: 12 August 2000     

Ra and Rn isotopes as natural tracers of submarine groundwater discharge in the patagonian coastal zone (Argentina): an initial assessment

Submarine groundwater discharge (SGD) is herein recognized as a significant pathway of material transport from land to the coastal SW Atlantic Ocean and thus, it can be a relevant factor affecting the marine biogeochemical cycles in the region. This paper focuses on the initial measurements of ²²⁶Ra, ²²⁸Ra and ²²²Rn made in Patagonia’s coastal zone of Chubut and Santa Cruz provinces (42°S–48°S, Argentina). ²²⁶Ra activity ranged from 2.9 to 73.5 dpm 100 L^?1, and ²²⁸Ra activity ranged from 11.9 to 311.0 dpm 100 L^?1 in groundwater wells. The radium activities found in Patagonia’s marine coastal regions and adjacent shelf indicate significant enrichment throughout the coastal waters. Groundwater samples presented the largest ²²²Rn activity and ranged from 2.66 to 1083 dpm L^?1. Conversely, in the coastal marine environment, the ²²²Rn activity ranged from 1.03 to 6.23 dpm L^?1. The Patagonian coastal aquifer showed a larger enrichment in ²²⁸Ra than in ²²⁶Ra, which is a typical feature for sites where SGD is dominant, probably playing a significant role in the biogeochemistry of these coastal waters.     

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.     

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.     

Radon-rich waters in Russia

In radon mineral curative waters, according to Russian mineral water classification, the radon concentration should be greater than 185 Bq/l. There are about 30 mineral waters with high levels of radon in Russia. Radon-rich waters have high therapeutic effects. It is proven that natural background radiation stimulates the human immune system. Radon is a natural radioactive gas that has no taste, smell or color. Radon-222 is one of the heaviest elements in the zero groups of inert gases. It is a gaseous radioactive element. All radon isotopes are -emitters while the transformation of its decay products is accompanied by the emitting of -or -particles. The main products of radon decay are short-lived isotopes Po, Pb, Bi, and TL. Belonging to the uranium and thorium decay chain, radon isotopes form directly during the decay of radium isotopes. Therefore the radon concentration depends upon the concentration of its parent's isotope in water and rocks washed by it as well as upon the amount of radon emanation. Loose rocks or rocks with a great number of cracks are characterized by higher radon concentration (zones of tectonic disturbance, weathering crusts, etc.).Crystalline rocks usually have higher uranium concentrations than the average bedrock. Examples of rock types, which often have enhanced uranium concentration >5% ppm U includes the following: granites, syenites, pegmatite, acid volcanic rocks and acid gneisses. In the earth's crust radon migrates either in a gaseous or dissolved state. It can go to the surface without any chemical reaction. Formation of the radon-rich therapeutics waters of Russia has been analyzed, and most of them are genetically connected to crystalline acid rocks that have exceeded uranium-radium mineralization. The radon content in Russia reaches more than 8,000 Bq/l. Radon-rich waters of this type occur in the Altai, Karelia, St Petersburg and Trans-Baikal regions. Another type is connected to geodynamic activity of regions and secondary radioactivity. A well-known example of radon-rich waters of the second type is Pyatigorsk in the North Caucasus. Mixing confined carbon dioxide-hydrogen sulfide water and unconfined groundwater forms radon waters. The radon concentration is 1,170–2,430 Bq/l. The occurrence of radon-rich water deposits in other regions of Russia is described. Further investigation of the radon content in other geological environments will contribute to the environmental safety as well as to the solution to many genetic, hydrogeochronological, paleoreconstructive and prediction problems in hydrogeology.     

Assessment of natural radioactivity in aquifer medium bearing uranium ores in Koprubasi,Turkey

Koprubasi, located within Manisa Province near the Izmir, is the biggest uranium mine where uranium ores originate from Neogene aged altered sandstone and conglomerate layers. The main objective of this study is to determine the radiation hazard associated with radioactivity levels of uranium ores, and the rocks and sediments around Koprubasi. In this regard, measured activity levels of ²²⁶Ra, ²³²Th and ⁴⁰K were compared with world averages. The average activity levels of ²²⁶ Ra, ²³²Th and ⁴⁰K were measured to be 5369.75, 124.78 and 10.0 Bq/kg in uranium ores, 24.32, 52.94 and 623.38 Bq/kg in gneiss, 46.24, 45.13 and 762.26 Bq/kg in sandstone and conglomerate, 73.11, 43.15 and 810.65 Bq/kg in sediments, respectively. All samples have high ²²⁶Ra and ⁴⁰K levels according to world average level. As these sediments are used as construction materials and in agricultural activities within the study area, the radiation hazard are calculated by using dose rate (D), annual effective dose rate (He), radium equivalent activity (Ra_eq) and radiation hazard index (I_yr). All the samples have Ra_eq levels that are lower than the world average limit of 370 Bq/kg. On the other hand, D, He and I_yr values are higher than world average values. These results indicate that the uranium ores in the Koprubasi is the most important contributor to the natural radiation level. The radioactivity levels of sediments and rocks make them unsuitable for use as agricultural soil and as construction materials. Moreover, it is determined that shallow groundwater in sediments and deep groundwater in conglomerate rocks and also surface water sources in the Koprubasi have high ²²⁶Ra content. According to environmental radioactive baseline, some environmental protection study must be taken in Koprubasi uranium site and the environment.     

The mobility of radium-226 and trace metals in pre-oxidized subaqueous uranium mill tailings

The exchange of ²²⁶Ra and trace metals across the tailings-water interface and the mechanisms governing their mobility were assessed via sub-centimetre resolution profiling of dissolved constituents across the tailings–water interface in Cell 14 of the Quirke Waste Management Area at Rio Algom's Quirke Mine, near Elliot Lake, Ontario, Canada. Shallow zones (<1.5 m water depth) are characterized by sparse filamentous vegetation, well-mixed water columns and fully oxygenated bottom waters. Profiles of dissolved O₂, Fe and Mn indicate that the tailings deposits in these areas are sub-oxic below tailings depths of ∼3 cm. These zones exhibit minor remobilization of Ra in the upper 5 cm of the tailings deposit; ²²⁶Ra fluxes at these sites are relatively small, and contribute negligibly to the water column activity of ²²⁶Ra. The shallow areas also exhibit minor remobilization of Ni, As, Mo and U. The release of these elements to the water cover is, however, limited by scavenging mechanisms in the interfacial oxic horizons. The presence of thick vegetation (Chara sp.) in the deeper areas (>2 m water depth) fosters stagnant bottom waters and permits the development of anoxia above the benthic boundary. These anoxic tailings are characterized by substantial remobilization of ²²⁶Ra, resulting in a relatively large flux of ²²⁶Ra from the tailings to the water column. The strong correlation between the porewater profiles of ²²⁶Ra and Ba (r²=0.99), as well as solubility calculations, indicate that the mobility of Ra is controlled by saturation with respect to a poorly ordered and/or impure barite phase [(Ra,Ba)SO₄]. In the anoxic zones, severe undersaturation with respect to barite is sustained by microbial SO₄ reduction. Flux calculations suggest that the increase in ²²⁶Ra activity in the water cover since 1995 (from <0.5 to 2.5 Bq l⁻¹) can be attributed to an increase in the spatial distribution of anoxic bottom waters caused by increased density of benthic flora. The anoxic, vegetated areas also exhibit minor remobilization with respect to dissolved As, Ni and Zn. The removal of trace metals in the anoxic bottom waters appears to be limited by the availability of free sulphide. Collectively, the data demonstrate that while the water cover over the U mill tailings minimizes sulphide oxidation and metal mobility, anoxic conditions which have developed in deeper areas have led to increased mobility of ²²⁶Ra.     

Assessing the solubility controls on vanadium in groundwater,northeastern San Joaquin Valley,CA

The solubility controls on vanadium (V) in groundwater were studied due to concerns over possible harmful health effects of ingesting V in drinking water. Vanadium concentrations in the northeastern San Joaquin Valley ranged from <3 μg/L to 70 μg/L with a median of 21 μg/L. Concentrations of V were highest in samples collected from oxic groundwater (49% > 25 μg/L) and lowest in samples collected from anoxic groundwater (70% < 0.8 μg/L). In oxic groundwater, speciation modeling (SM) using PHREEQC predicted that V exists primarily as the oxyanion H₂VO₄⁻. Adsorption/desorption reactions with mineral surfaces and associated oxide coatings were indicated as the primary solubility control of V⁵⁺ oxyanions in groundwater. Environmental data showed that V concentrations in oxic groundwater generally increased with increasing groundwater pH. However, data from adsorption isotherm experiments indicated that small variations in pH (7.4–8.2) were not likely as an important a factor as the inherent adsorption capacity of oxide assemblages coating the surface of mineral grains. In suboxic groundwater, accurate SM modeling was difficult since Eh measurements of source water were not measured in this study. Vanadium concentrations in suboxic groundwater decreased with increasing pH indicating that V may exist as an oxycationic species [e.g. V(OH)₃⁺]. Vanadium may complex with dissolved inorganic and organic ligands under suboxic conditions, which could alter the adsorption behavior of V in groundwater. Speciation modeling did not predict the existence of V-inorganic ligand complexes and organic ligands were not collected as part of this study. More work is needed to determine processes governing V solubility under suboxic groundwater conditions. Under anoxic groundwater conditions, SM predicts that aqueous V exists as the uncharged V(OH)₃ molecule. However, exceedingly low V concentrations show that V is sparingly soluble in anoxic conditions. Results indicated that V may be precipitating as V³⁺- or mixed V³⁺/Fe³⁺-oxides in anoxic groundwater, which is consistent with results of a previous study. The fact that V appears insoluble in anoxic (Fe reducing) redox conditions indicates that the behavior of V is different than arsenic (As) in aquifer systems where the reductive dissolution of Fe-oxides with As adsorbed to the surface is a well-documented mechanism for increasing As concentrations in groundwater. This hypothesis is supported by the relation of V to As concentrations in oxic versus anoxic redox conditions.Sequential extraction procedures (SEP) applied to aquifer material showed that the greatest amount of V was recovered by the nitric acid (HNO₃) extract (37–71%), followed by the oxalate-ascorbic acid extract (19–60%) and the oxalate extract (3–14%). These results indicate that V was not associated with the solid phase as an easily exchangeable fraction. Although the total amount of V recovered was greatest for the HNO₃ extract that targets V adsorbed to sorption sites of crystalline Al, Fe and Mn oxides, the greatest V saturation of sorption sites appeared to occur on the amorphous and poorly crystalline oxide solid phases targeted by the oxalate and oxalate-ascorbic acid extracts respectively. Adsorption isotherm experiments showed no correlation between V sorption and any of the fractions identified by the SEP. This lack of correlation indicates the application of an SEP alone is not adequate to estimate the sorption characteristics of V in an aquifer system.     

The Role of Ocean Tides on Groundwater-Surface Water Exchange in a Mangrove-Dominated Estuary: Shark River Slough,Florida Coastal Everglades,USA

Low-relief environments like the Florida Coastal Everglades (FCE) have complicated hydrologic systems where surface water and groundwater processes are intimately linked yet hard to separate. Fluid exchange within these low-hydraulic-gradient systems can occur across broad spatial and temporal scales, with variable contributions to material transport and transformation. Identifying and assessing the scales at which these processes operate is essential for accurate evaluations of how these systems contribute to global biogeochemical cycles. The distribution of ²²²Rn and ^223,224,226Ra have complex spatial patterns along the Shark River Slough estuary (SRSE), Everglades, FL. High-resolution time-series measurements of ²²²Rn activity, salinity, and water level were used to quantify processes affecting radon fluxes out of the mangrove forest over a tidal cycle. Based on field data, tidal pumping through an extensive network of crab burrows in the lower FCE provides the best explanation for the high radon and fluid fluxes. Burrows are irrigated during rising tides when radon and other dissolved constituents are released from the mangrove soil. Flushing efficiency of the burrows—defined as the tidal volume divided by the volume of burrows—estimated for the creek drainage area vary seasonally from 25 (wet season) to 100 % (dry season) in this study. The tidal pumping of the mangrove forest soil acts as a significant vector for exchange between the forest and the estuary. Processes that enhance exchange of O₂ and other materials across the sediment-water interface could have a profound impact on the environmental response to larger scale processes such as sea level rise and climate change. Compounding the material budgets of the SRSE are additional inputs from groundwater from the Biscayne Aquifer, which were identified using radium isotopes. Quantification of the deep groundwater component is not obtainable, but isotopic data suggest a more prevalent signal in the dry season. These findings highlight the important role that both tidal- and seasonal-scale forcings play on groundwater movement in low-gradient hydrologic systems.     

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.     

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.     

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.