Natural colloids and suspended particles in the Whiteshell Research Area,Manitoba, Canada,and their potential effect on radiocolloid formation

Natural colloids (1–450 nm) and suspended particles (>450 nm) were characterized in groundwaters of the Whiteshell Research Area of southern Manitoba to evaluate their potential role in radionuclide transport through fractured granite. Data on particle concentrations, size distributions, compositions and natural radionuclide content were collected to predict radionuclide formation and to provide a database for future colloid migration studies. The concentrations of colloids between 10 and 450 nm ranged between 0.04 and 1 mg/l. The concentrations of suspended particles, which require higher groundwater velocities for transport, varied from 0.04 to 14 mg/l. Colloid (10–450 nm) concentrations as low as these observed in Whiteshell Research Area groundwater would have a minimal effect on radionuclide transport, assuming that radionuclide sorption on colloids is reversible. If radiocolloid formation is not reversible, and radionuclide-containing colloids cannot sorb onto fracture walls, the importance of natural colloids in radionuclide transport will depend upon particle migration properties.     

Chemical and physical characterization of suspended particles and colloids in waters from the Osamu Utsumi mine and Morro do Ferro analogue study sites, Poços de Caldas, Brazil

Data are presented on suspended particles and colloids in groundwaters from the Osamu Utsumi mine and the Morro do Ferro analogue study sites. Cross-flow ultrafiltration with membranes of different pore sizes (450 nm to 1.5 nm) was used to prepare colloid concentrates and ultrafiltrates for analyses of major and trace elements and U- and Th-isotopic compositions. Additional characterization of colloidal and particulate material was performed by ESCA, SEM and X-ray diffraction. The results indicate the presence of low concentrations of colloids in these waters (typically < 500 μg/l), composed mainly of iron/organic species. Minor portions of uranium and other trace elements, but significant fractions of the total concentrations of Th and REE in prefiltered waters (< 450 nm) were associated with these colloids.Suspended particles (> 450 nm), also composed mainly of hydrous ferric oxides and humic-like compounds, show the same trend as the colloids with respect to U, Th and REE associations, but elemental concentrations were typically higher by a factor of 1,000 or more. In waters of low pH and with high sulphate content, these associations are considerably lower. Due to the low concentrations of suspended particles in groundwaters from the Osamu Utsumi uranium mine (typically <0.5 mg/l), these particles carry only a minor fraction of U and the REE (<10% of the total concentrations in unfiltered groundwaters), but a significant, usually predominant fraction of Th (30–70%). The suspended particle load in groundwaters from the Morro do Ferro environment is typically higher than in those from the mine by a factor of 5 to 10. This suggests that U, Th and the REE could be transported predominantly by particulate matter. However, these particles and colloids seem to have a low capacity for migration.     

Stability assessment and characterization of colloids in coastal groundwater aquifer system at Kalpakkam

Natural colloids have a potential role in facilitating the transport of radionuclides in groundwater. To assess the role of mobile colloidal phases in radionuclide transport, characterization of colloids for size, size distribution, zeta potential, surface charge and elemental composition is required. Groundwater samples were collected from 12 borewells in the study area and were characterized with respect to physicochemical parameters. Water quality parameters such as pH, temperature, specific conductance, TDS and dissolved O₂ were measured in situ. Based on salinity, two groundwater types were identified in the study area: (1) freshwater type and (2) brackish type. Laboratory and field-scale turbidity measurements in addition to quantitative analysis of major ions were carried out. It was observed that the colloid concentrations are reduced at higher salinity. Zetasizer, particle size analyzer, scanning electron microscopy, energy dispersive X-ray analysis and X-ray diffraction techniques were used to characterize the colloidal particles in groundwater. Colloids were present in all the groundwater samples, the concentration varying between 0.05 and 6 mg/L. Colloid concentration was greater in wells with low ionic strength and the number of colloidal particles varied between 3 × 10⁹ and 4 × 10¹¹ particles/L. The average colloid size varied between 200 and 350 nm for various samples. The zeta potential of the colloidal particles varied between −25.5 and –34.0 mV. SEM analysis of colloidal particles revealed the presence of clays particularly kaolinite and that the mineral composition of colloids reflects the mineralogy of the aquifer. For proper risk assessment and remediation studies, the role of colloids in radionuclide transport assumes greater importance. This study highlights the need for, and relevance of, detailed colloid characterization to assess its role in the migration of radionuclides from near surface disposal facilities.     

High levels of uranium and radium in groundwaters at Canada's Underground Research Laboratory, Lac du Bonnet, Manitoba, Canada

High concentrations of U and²²⁶Ra, and elevated²³⁴U/²³⁸U activity ratios have been measured in groundwater samples collected from water supply wells and exploratory boreholes in the area surrounding the Underground Research Laboratory (URL) of Atomic Energy of Canada Limited, in southeastern Manitoba. All groundwaters come from the Lac du Bonnet granite batholith or sediments overlying the batholith.Uranium concentrations attain almost 1 mg/l in some shallow, low-salinity groundwaters, whereas²²⁶Ra tends to be high (up to 38 Bq/l) in deeper, saline waters. The U concentrations are some of the highest observed in global groundwaters, yet no significant ore body or mineralization is known in the area. Analyses of unaltered rock samples of the Lac du Bonnet granite show slight U enrichment over average Canadian Shield granites (6.5 μg/g vs 4 μg/g), and altered wall rock in fracture zones is enriched in U by up to an order of magnitude compared to adjacent bedrock. Low²³⁴U/²³⁸U activity ratios in this altered rock indicate active and recent leaching of U by groundwater.The key control on U concentration appears to be redox potential. Concentrations of U in rock, residence time and groundwater composition are of lesser importance. Geochemical modelling of the shallower, oxidized waters indicates that U speciation consists mainly of anionic carbonate complexes of the uranyl ion. This is supported by the remarkable efficiency of an anionic filter developed to remove high levels of U from drinking water in the area.In more reducing groundwaters, U concentrations are similar to those determined in recent experimental work on uraninite solubility in the pH range 7–8.5. Colloidal U is <10% of total U and organic complexation is unlikely to be significant because of low dissolved organic concentrations. The results emphasize the significance of redox potential in controlling U mobility in both oxidizing and reducing environments and indicate the usefulness of U concentration in estimating groundwater Eh.     

Characterization of organics in whiteshell research area groundwater and the implications for radionuclide transport

Naturally occurring organics in groundwaters of the Whiteshell Research Area (WRA) of southern Manitoba were investigated to assess their potential role in radionuclide transport within granite fractures of the Canadian Shield. A survey of dissolved organic carbon concentrations, carried out to determine the variability in the organic content of these groundwaters, showed average concentrations of 0.8 ± 0.1 mg/L for Fracture Zone 2, 0.8 ± 0.4 mg/L for near-vertical fractures and 2.3 ± 0.8 mg/L for deeper saline groundwater. The dissolved organic carbon consisted mainly of hydrophilic neutral compounds (60 to 75%), and hydrophobic and hydrophilic acids (23 to 39%), along with very small amounts of hydrophobic bases and neutrals, and hydrophilic bases. Significant contamination from drilling operations and plastics, mostly in the form of hydrophobic neutrals, was observed in some samples. These compounds would not contribute to radionuclide migration in a natural system and are not included in the assessment of the organic complexing capacity of these groundwaters.Based on groundwater concentrations of hydrophobic and hydrophilic acids and on the measured car☐ylic functional group content of these acids, the average complexing capacity of natural organics in Whiteshell Research Area groundwaters was calculated to be 2.9 × 10⁻⁶ eq/L. The ability of these organics to complex radionuclides was tested using conditional stability constants from the literature for humic complex formation with Am(III), Th(IV), and U(VI). The chemistry of U(VI) was predicted to be dominated by inorganic complexes and not significantly affected by organics. The literature contains a wide range in values of stability constants for Am(III) and Th(IV) complexes with humics. The aqueous chemistry of Am(III) and Th(VI) could be affected by complexation with natural organics if the higher stability constant values are valid for WRA groundwaters.     

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.     

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.     

两花岗岩体接触带铀系核素迁移的初步模拟

随着世界各国大力发展核电，放射性废料的安全处置已成为当今研究热点和前沿学科。高放废物深地质处置的安全性主要取决于处置库内放射性核素向生物圈的迁移程度。在侵入岩中，放射性核素主要是通过地下水沿岩石孔隙从处置库向生物圈迁移的。为了理解放射性核素在花岗岩体接触带的迁移行为，本文根据两花岗岩体接触带中样品的铀系核素放射性活度比值（^234U/^238U,^230Th/^234U,^226Ra/^230Th,^230Th/^238U)，利用 α-反冲（弹射）作用引起的放射性不平衡理论，计算了铀系核素子体^234U,^230Th,^226Ra在后期地下水的作用下在花岗岩体接触带及其裂隙内的迁出率、迁入率、并进行了质量平衡的计算。结果表明，经α-反冲作用进入流体的核素的迁出率要远大于因核素自然衰变的消亡率；裂隙充填物及裂隙能阻滞大量核素的迁移，其沉淀核素来自接触带花岗岩；花岗岩能强烈阻滞核素的迁移，可作为阻止放射性核素从核废料地下处置库向外迁移的有利天然屏障。     

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.     

Mineral chemistry and oxygen isotopic analyses of uraninite,pitchblende and uranium alteration minerals from the Cigar Lake deposit,Saskatchewan, Canada

The Cigar Lake unconformity-type U deposit is one of the largest and highest grade U deposits in the Proterozoic Athabasca Basin, northern Saskatchewan, Canada. Cigar Lake has recently been the focus of an international, 3-a, collaborative program in which this U deposit was studied as a natural analogue for a spent nuclear fuel repository. The deposit is located near the eastern margin of the Athabasca Basin, 430 m below the surface, at the intersection between Hudsonian-age faults and the unconformity between Athabasca group sandstones and Aphebian metasediments. Three stages of U mineralization have been identified based on cross-cutting relationships and textures observed in thin section and back-scattered electron (BSE) images, O isotope data and chemical compositions. All stages of U mineralization have been variably altered to Ca-rich, U-hydrate minerals or uranyl oxide hydrate minerals and coffinite.UPb chemical ages of the 3 stages of U mineralization from Cigar Lake coincide with the 3 major fluid events that precipitated clay and silicate minerals at 1500 Ma, 950 Ma, and 300 Ma, throughout the entire Athabasca Basin. Stage 1 and 2 uraninite and pitchblende have the lowest δ¹⁸O values that range from −30.1 ‰ to −15.2‰; whereas, stage 3 uraninite has δ¹⁸O values ranging from −10.0‰ to −3.4‰. Uranyl oxide hydrate minerals have δ¹⁸O values that range from −11.3‰ to −8.2‰; whereas, uranyl minerals have much higher δ¹⁸O values. Based on UPb chemical ages,δ¹⁸O values, and petrographic relationships of U alteration minerals associated with primary U mineralization, the Cigar Lake U ore is similar to U ore from other unconformity-type U deposits in the Athabasca Basin. Therefore, the Cigar Lake ore deposit, although surrounded by clay and sandstone barriers, has been effected by the same fluid events that have altered other unconformity-type U deposits in the Athabasca Basin.The 3 stages of ore formation and associated alteration minerals permit the detailed study of fluids responsible for U deposition and alteration. This information provides the necessary context for the evaluation of the Cigar Lake deposit as a “natural analogue” for the disposal of spent nuclear fuel in underground vaults in rocks of the Canadian Shield.     

Transport of colloidal contaminants in groundwater: radionuclide migration at the Nevada test site

Large-volume groundwater samples were collected at the Nevada Test Site from within a nuclear detonation cavity and from approximately 300 m outside the cavity. The samples were filtered and ultrafiltered, and the filtrates and various particle size fractions were analyzed for chemical composition and radionuclide activity. In samples from both locations, approximately 100% of the transition element (Mn, Co) and lanthanide (Ce, Eu) radionuclides were associated with colloids. Their presence outside the cavity indicates transport in the colloidal form. Distribution coefficients calculated for Ru, Sb, and Cs nuclides from both field sample locations indicate equilibrium partitioning on the 0.05-0.003 μm colloids. Calculation of transport efficiencies relative to colloid mass concentrations and dissolved neutral or anionic nuclides indicates that both the cations and the radiolabelled colloids appear to experience capture by or exchange with immobile aquifer surfaces.     

Effects of human-induced alteration of groundwater flow on concentrations of naturally-occurring trace elements at water-supply wells

The effects of human-induced alteration of groundwater flow patterns on concentrations of naturally-occurring trace elements were examined in five hydrologically distinct aquifer systems in the USA. Although naturally occurring, these trace elements can exceed concentrations that are considered harmful to human health. The results show that pumping-induced hydraulic gradient changes and artificial connection of aquifers by well screens can mix chemically distinct groundwater. Chemical reactions between these mixed groundwaters and solid aquifer materials can result in the mobilization of trace elements such as U, As and Ra, with subsequent transport to water-supply wells. For example, in the High Plains aquifer near York, Nebraska, mixing of shallow, oxygenated, lower-pH water from an unconfined aquifer with deeper, confined, anoxic, higher-pH water is facilitated by wells screened across both aquifers. The resulting higher-O₂, lower-pH mixed groundwater facilitated the mobilization of U from solid aquifer materials, and dissolved U concentrations were observed to increase significantly in nearby supply wells. Similar instances of trace element mobilization due to human-induced mixing of groundwaters were documented in: (1) the Floridan aquifer system near Tampa, Florida (As and U), (2) Paleozoic sedimentary aquifers in eastern Wisconsin (As), (3) the basin-fill aquifer underlying the California Central Valley near Modesto (U), and (4) Coastal Plain aquifers of New Jersey (Ra). Adverse water-quality impacts attributed to human activities are commonly assumed to be related solely to the release of the various anthropogenic contaminants to the environment. The results show that human activities including various land uses, well drilling, and pumping rates and volumes can adversely impact the quality of water in supply wells, when associated with naturally-occurring trace elements in aquifer materials. This occurs by causing subtle but significant changes in geochemistry and associated trace element mobilization as well as enhancing advective transport processes.     

Controls on the geochemistry of rare earth elements along a groundwater flow path in the Carrizo Sand aquifer,Texas, USA

Groundwater samples were collected along a groundwater flow path in the Carrizo Sand aquifer in south Texas, USA. Field measurements that included pH, specific conductivity, temperature, dissolved oxygen (DO), oxidation–reduction potentials (Eh in mV), alkalinity, iron speciation, and H₂S concentrations were also conducted on site. The geochemistry (i.e., concentrations, shale-normalized patterns, and speciation) of dissolved rare element elements (REEs) in the Carrizo groundwaters are described as a function of distance along a flow path. Eh and other redox indicators (i.e., DO, Fe speciation, H₂S, U, and Re) indicate that redox conditions change along the flow path in the Carrizo Sand aquifer. Within the region of the aquifer proximal to the recharge zone, groundwaters exhibit both highly oxidizing and localized mildly reducing conditions. However, from roughly 10 km to the discharge zone, groundwaters are reducing and exhibit a progressive decrease in redox conditions. Dissolved REE geochemical behavior exhibits regular variations along the groundwater flow path in the Carrizo Sand aquifer. The changes in REE concentrations, shale-normalized patterns, and speciation indicate that REEs are not conservative tracers. With flow down-gradient, redox conditions, pH and solution composite, and adsorption modify groundwater REE concentrations, fractionation patterns, and speciation.     

234Th/238U不平衡法在真光层颗粒动力学研究中的应用

真光层是海洋浮游生物活动最为活跃的区域,其间发生的颗粒动力学过程及其机制对于海洋碳的生物地球化学循环有着重要影响,利用放射性核素示踪海洋真光层颗粒动力学过程成为近年来海洋科学的前沿课题。介绍了该领域＾２３４Ｔｈ－＾２３８Ｕ不平衡法的原理、发展历程及其在ＰＯＣ输出通量的估算、沉积物捕集器捕集效率的校正、真光层层化结构的揭示、颗粒活性元素固／液界面分配机制的研究、海洋胶体性质的研究及近岸海域悬浮颗粒活     

Migration of Some Elements and Radionuclides across aGranite-Granite Contact Zone: A Natural Analoguefor Safe Disposal of High-Level Radwastes

Elements and natural radionuclides in the contact zone of two granites with different ages would migrate from one to the other because of the difference in their chemical contents and later water-rock interactions. This migration could serve as an analogue for the near-field process of radwastes in a high-level radwaste deep geological disposal repository.In the contact between the Indosinian granite (whole-rock Rb-Sr isochron age at 214@3 Ma) and Hercynian granite (zircon U-Pb isochron age at 296@31 Ma) located in Ziyuan County, Guangxi, the O and Pb isotope characteristics and the activity ratios of 234U/238U, 230Th/238U, 230Th/234U and 226Ra/230Th show that, based on the whole-rock chemical contents, both of the two granites have maintained a relatively open chemical system in their evolution processes. However, as there is no obvious open fault, the migration of major elements, trace elements and natural U-series nu-clides takes place within only 1-2 m in the contact zone, and water-rock interaction     

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.     

Mobilisation of arsenic and other trace elements in fluviolacustrine aquifers of the Huhhot Basin,Inner Mongolia

Observed As concentrations in groundwater from boreholes and wells in the Huhhot Basin of Inner Mongolia, northern China, range between <1 μg l⁻¹ and 1480 μg l⁻¹. The aquifers are composed of Quaternary (largely Holocene) lacustrine and fluvial sediments. High concentrations are found in groundwater from both shallow and deep boreholes as well as from some dug wells (well depths ranging between <10 m and 400 m). Populations from the affected areas experience a number of As-related health problems, the most notable of which are skin lesions (keratosis, melanosis, skin cancer) but with internal cancers (lung and bladder cancer) also having been reported. In both the shallow and deep aquifers, groundwaters evolve down the flow gradient from oxidising conditions along the basin margins to reducing conditions in the low-lying central part of the basin. High As concentrations occur in anaerobic groundwaters from this low-lying area and are associated with moderately high dissolved Fe as well as high Mn, NH₄, dissolved organic C (DOC), HCO₃ and P concentrations. Many of the deep groundwaters have particularly enriched DOC concentrations (up to 30 mg l⁻¹) and are often brown as a result of the high concentrations of organic acid. In the reducing groundwaters, inorganic As(III) constitutes typically more than 60% of the total dissolved As. The highest As concentrations tend to be found in groundwater with low SO₄ concentrations and indicate that As mobilisation occurs under strongly reducing conditions, where SO₄ reduction has been an active process. High concentrations of Fe, Mn, NH₄, HCO₃ and P are a common feature of reducing high-As groundwater provinces (e.g. Bangladesh, West Bengal). High concentrations of organic acid (humic, fulvic acid) are not a universal feature of such aquifers, but have been found in groundwaters from Taiwan and Hungary for example. The observed range of total As concentrations in sediments is 3–29 mg kg⁻¹ (n=12) and the concentrations correlate positively with total Fe. Up to 30% of the As is oxalate-extractable and taken to be associated largely with Fe oxides. The release of As into solution under the reducing conditions is believed to be by desorption coupled with reductive dissolution of the Fe oxide minerals. The association of dissolved As with constituents such as HCO₃, DOC and P may be a coincidence related to the prevalent reducing conditions and slow groundwater flow, but they may also be directly involved because of their competition with As for binding sites on the Fe oxides. The Huhhot groundwaters also have some high concentrations of dissolved U (up to 53 μg l⁻¹) and F⁻ (up to 6.8 mg l⁻¹). In contrast to As, U occurs predominantly under the more oxidising conditions along the basin margins. Fluoride occurs dominantly in the shallow groundwaters which have Na and HCO₃ as the dominant ions. The combination of slow flow of groundwater and the young age of the aquifer sediments are also considered potentially important causes of the high dissolved As concentrations observed as the sediments are likely to contain newly-formed and reactive minerals and have not been well flushed since burial.     

Distribution of natural uranium,thorium, lead,and polonium radionuclides in tidal phases of a Delaware salt marsh

Natural radionuclides in the uranium and thorium series were measured in solid tidal phases (suspended particles, bottom sediment, surface microlayer colloids) of a salt marsh in lower Delaware. The purpose was to identify potential processes responsible for trace element cycling (sources, redistribution and exchange) in salt water marshes and with their coastal waters. Generally, concentrations of U, Th,²¹⁰Pb, and²¹⁰Po on the tidal solid phases suggest a general mechanism by which tidal marshes appear to be trapping the nuclides into their interiors. The processes may include transport of enriched fine particles into the marsh, capture by salt marsh grass and chemical fixation by redox processes at the sediment surface. Specifically, the uranium contents of most of the samples are similar with activity ratios²³⁴U²³⁸U≧1, indicating a mixture of detrital and nondetrital (authigenic) uranium inputs such as seawater or ground water. Since the²³⁰Th daughter is generally deficient by about 50%, the authigenic enrichment process appears to favor uranium and is potentially linked to the extensive diagenetic sulfur redox cycle of salt marsh sediments. The²¹⁰Po/²¹⁰Pb activity ratio is less than one on Spartina adsorbed solids, and could suggest a general process in salt marshes which favors²¹⁰Pb enrichment by atmospheric fallout over enrichment of²¹⁰Po on time scales of weeks which correspond to complete tide marsh exchange. A²²⁸Th/²³²Th activity ratio of less than unity on the solids adsorbed onto marsh grass suggests a net process whereby diffusive loss of the intermediate daughter²²⁸Ra from the adsorbed solids to tidal waters dominates over potential²²⁸Th scavenging by suspended sediment.     

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.     

Trace element mobility in mine waters from granitic pegmatite U–Th–REE deposits,Bancroft area,Ontario

Small, low-grade, granitic pegmatite U–Th–REE deposits are found throughout the Grenville geological province of eastern Canada. Groundwater quality at historical mining properties in the Bancroft area was investigated in order to better understand the mobility of trace elements that may pose health risks if there is renewed development of this class of mineral deposit. Groundwater samples were obtained from diamond drill holes, flowing adits and flooded mine shafts. Uranium occurs almost entirely in the dissolved (<0.45 μm) phase and is found at concentrations reaching 2579 μg/L. The Canadian maximum acceptable concentration for U in drinking water (0.02 mg/L) was exceeded in 70% of samples. Regulatory limits for ²²⁶Ra (0.5 Bq/L) and for ²¹⁰Pb (0.2 Bq/L) were generally exceeded in these samples as well. Speciation modeling indicates that over 98% of dissolved U is in the form of highly mobile uranyl-Ca–carbonate complexes known to inhibit U adsorption. Uranium concentrations in groundwater appear to be correlated with the uranothorite content of the deposits rather than with their U grade. Uranothorite may be more soluble than uraninite, the other ore mineral, because of its non-ideal composition and metamict structure. Thorium, released concomitantly with U during the dissolution of uranothorite and thorian uraninite, exhibits median and maximum total concentrations of only 0.1 and 11 μg/L, respectively. Mass balance and stoichiometric considerations indicate that almost all Th is immobilized very close to its source. The sums of total light REE (La–Gd) concentrations have median and maximum values of 6 and 117 μg/L, respectively. The sums of total heavy REE (Tb–Lu) concentrations have median and maximum values of 0.8 and 21 μg/L, respectively. Light REE are derived mainly from the dissolution of metamict allanite whereas the sources of heavy REE are widely dispersed among accessory minerals. Fractionation patterns of REE in the dissolved phase are flat or concave, with negative Ce anomalies associated with more oxic groundwaters. The data suggest preferential LREE and HREE complexation with organic and carbonate ligands in the dissolved phase, respectively. Fractionation patterns in the suspended particulate phase exhibit decreasing enrichment with atomic number from La to Gd and a flat profile from Tb to Lu. This is explained by preferential sorption of LREE and uniform sorption of HREE. Manganese particulates are the most likely sorbents. Potential health risks from Th or REE in mine waters are unlikely due to the very low mobility of these elements. Uranium, on the other hand, exhibits high mobility in shallow, oxic groundwaters and drainage from some mine adits may require mitigation.