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1.
The chemical, isotopic and mineralogical alteration which occurred during primary uranium ore deposition at the breccia pipe-hosted Osamu Utsumi mine, Poços de Caldas, Brazil was studied as a natural analogue for near field radionuclide migration. Chemical and isotopic alteration models were combined with finite difference models of the convective cooling of caldera intrusives. The modeling indicates that the intense chemical, isotopic, and mineralogical alteration of the Osamu Utsumi breccia pipe requires the circulation of > 105 kg/cm2 of boiling hydrothermal fluid > 200°C through each square centimeter cross-section of the pipe. This circulation could be driven by heat from a 6 km diameter intrusive extending to 10 km depth. Even with this large amount of circulation concentrated in the permeable breccia pipe, uranium solubilities must be orders of magnitude greater than indicated in the most recent experiments (and more in line with previous estimates) to produce the primary uranium mineralization at the Osamu Utsumi mine.The same models applied to a hypothetical high temperature waste repository show that heat from radioactive decay will produce a hydrothermal circulation system remarkably similar to that studied at the natural analogue site at Poços de Caldas. The depth of fluid convection induced by the hypothetical repository would be 5 to 10 km, the maximum temperature would be 300°C, the lifetime of the high temperature phase would be a few thousand years, and boiling would occur and cause most of the alteration within the hypothetical waste repository. This physical analysis emphasizes the importance of permeability on a 10 × 10 × 10 km scale in controlling the potential amount of circulation through the hypothetical repository.Application of the chemical models successfully used to interpret mineralization and alteration at the Poços de Caldas Osamu Utsumi mine to the hypothetical waste repository shows that even in a worst case scenario (waste implaced in a permeable host rock with no measures taken to inhibit flow though the repository) the amount of hydrothermal alteration in the hypothetical repository will be 0.1% of that in the breccia pipe at Osamu Utsumi. Assuming no barriers to uranium mobility, uranium precipitation above the hypothetical repository would be 0.04 ppm (rather than 40 ppm), hydrothermal alteration 0.03 wt% (rather than 30 wt%), etc.Our analysis indicates that modeled mineralogical alteration is sensitive to the thermodynamic data base used. Prediction of mineralogical alteration (which may be necessary to predict the migration of radionuclides other than uranium, for example) probably cannot be based directly on even very carefully collected laboratory thermodynamic data. Mineralogical complexities of the system, as well as data base uncertainties will require calibration of the thermodynamic framework against mineralogical alteration observed in the laboratory or field.  相似文献   

2.
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3.
Leach tests carried out on tektite specimens (indochinites and australites) under high-dilution conditions show a common behavior characterized by low leach rates (1.8 × 10?5g · m?2 · d?1or 7.2 × 10?12m · d?1 at 23°C) and an activation energy of (79.6 ± 0.7) × 103J · mol?1. The extent of selective leaching is very small, of the order of 10?8 m. Extrapolation of test results over the lifetime of the tektites gives an excellent agreement with field observations on the extent of corrosion, and this is an important step in establishing the validity of laboratory tests as a basis for the development of models and predictions concerning long-term durabilities at least in the limiting case of high dilution or rapid flow. The results are also shown to be in agreement with various previous observations on the corrosion resistance of tektites. The chemical durability of tektites is observed to be consistent with their composition, highlighting requirements for high corrosion resistance in glasses; these requirements include a silica content in excess of 67 mol%, an extremely low water content and an alkali content which is low both absolutely and relative to the di- and poly-valent metal oxide levels. It is shown that artificial glasses which fulfil these criteria are no less corrosion-resistant than the corresponding natural glasses. These conclusions have bearing on the development as well as on the evaluation of glasses intended for very long service, such as radioactive waste vitrification media.  相似文献   

4.
To improve confidence in glass alteration models, as used in nuclear and natural applications, their long-term predictive capacity has to be validated. For this purpose, we develop a new model that couples geochemical reactions with transport and use a fractured archaeological glass block that has been altered for 1800 years under well-constrained conditions in order to test the capacity of the model.The chemical model considers three steps in the alteration process: (1) formation of a hydrated glass by interdiffusion, whose kinetics are controlled by a pH and temperature dependent diffusion coefficient; (2) the dissolution of the hydrated glass, whose kinetics are based on an affinity law; (3) the precipitation of secondary phases if thermodynamic saturation is reached. All kinetic parameters were determined from experiments. The model was initially tested on alteration experiments in different solutions (pure water, Tris, seawater). It was then coupled with diffusive transport in solution to simulate alteration in cracks within the glass. Results of the simulations run over 1800 years are in good agreement with archaeological glass block observations concerning the nature of alteration products (hydrated glass, smectites, and carbonates) and crack alteration thicknesses. External cracks in direct contact with renewed seawater were altered at the forward dissolution rate and are filled with smectites (400−500 μm). Internal cracks are less altered (by 1 or 2 orders of magnitude) because of the strong coupling between alteration chemistry and transport. The initial crack aperture, the distance to the surface, and sealing by secondary phases account for these low alteration thicknesses. The agreement between simulations and observations thus validates the predictive capacity of this coupled geochemical model and increases more generally the robustness and confidence in glass alteration models to predict long-term behavior of nuclear waste in geological disposal or natural glass in the environment.  相似文献   

5.
《Applied Geochemistry》1998,13(1):105-126
Leaching experiments in aqueous media were carried out on non-radioactive and radioactive nuclear waste glasses to investigate the release behaviour of 4 actinides (Th, U, Np and Pu) and 3 lanthanides (La, Ce and Nd) from the solid into solution. The experiments were conducted under flowing conditions using synthetic aqueous solutions. The lanthanide and actinide concentrations were measured in the leachates before and after filtration to 0.45 μm and 1.8 nm.Over 98.5% of the lanthanides and Th released from the glass were retained in the alteration products on the glass surface, probably coprecipitated with a siliceous gel. The retention was enhanced by the presence in the gel of 20 wt% P oxides from the initial 5 × 10−3 M PO4 solution. In the leachates, more than 90% of the lanthanides and Th were associated with colloidal particles.Uranium and Np retention varied from 40% in a 5 × 10−3 M CO3 medium to 95% in a 5 × 10−3 M PO4 medium. In the CO3 medium, U and Np formed stable CO3 complexes that diminished the formation of precipitates; in the PO4 medium, precipitation of PO4 or more complex phases may have occurred.Pu exhibited atypical behaviour to the extent that it was strongly bonded to colloidal particles in solution, concentrated in the fraction exceeding 0.45 μm, and modifyed the calculated Pu leach rates. These particles may be the result of limited disaggregation of the alteration film. As most of the Pu was found at valence IV, it may be strongly retained in the alteration layer by precipitation or coprecipitation.Under oxidizing conditions, Np and U are found at high valences as Np(V) and U(VI), yielding charged forms in solution (NpO2+ and UO2+). The lanthanides, Th and Pu were present at lower valences as Ln(III), Th(IV) and Pu(IV), yielding Ln3+, Th4+ and Pu4+ in oxidizing media. The different behaviour of U and Np compared with the lanthanides, Th or Pu, observed during these experiments shows that the valence is the determining factor, and must be taken into account in assessing the evolution of radionuclides during the alteration of nuclear waste glass.  相似文献   

6.
Interactions between nuclear glass and Fe were investigated in a clayey environment to better understand the mechanisms and driving forces controlling the long-term behavior of high-level waste glass in a geological repository. An integrated experiment involving a Glass–Iron–Clay (GIC) stack was run at a laboratory scale in anoxic conditions for 2 years and the interfaces were characterized by a multiscale approach using scanning electron microscopy coupled with energy dispersive spectroscopy, transmission electron microscopy, Raman microspectroscopy and scanning transmission X-ray microscopy at the SLS Synchrotron. The characterization of glass alteration patterns on cross sections revealed an increase in glass alteration with the Fe content and the proximity between the glass and Fe. The alteration layers are polyphase and stratified with an inner porous gel layer incorporating Fe and an outer layer composed of nanocrystalline Fe-silicates. Several mechanisms which could affect the glass alteration kinetics and the transport properties of the alteration layer are proposed to explain this pattern: (i) consumption of hydrolyzed silica by precipitation of Fe-silicates; (ii) penetration of Fe within the gel porosity probably as precipitates such as Fe oxyhydroxide or Fe-silicates. These new data may imply some consequences when considering the long-term behavior of glass in geological disposal conditions.  相似文献   

7.
The minimum age of a zone of secondary uranium mineralization, located at the Austatom Prospect in the Alligator Rivers region of Australia, is estimated to be 3.6 × 105y. This is derived from a geochronological model based on retarded leaching of 234U with respect to 238U and on ratios within the ore of these members of the 238U decay series. Although kaolinite is a dominant mineral in the weathered schist-host-rocks, retarded dissolution of 234U occurs only in the presence of the clay minerals illite and montmorillonite. In their absence the reverse occurs. A model is proposed to explain the results. Ratios of 230Th to 238U indicate that the mineralization has probably remained stationary within the weathered schist for at least 1 to 2 × 105y. Future use of clay minerals as buffers in radioactive waste repositories is supported by the excellent long-term retention obtained for oxidized uranium, probably due in part to isomorphic substitution into the clay crystal lattice.  相似文献   

8.
Data from studies of dissimilatory bacterial (108 cells mL−1 of Shewanella putrefaciens strain CN32, pH 6.8) and ascorbate (10 mM, pH 3.0) reduction of two synthetic Fe(III) oxide coated sands and three natural Fe(III) oxide-bearing subsurface materials (all at ca. 10 mmol Fe(III) L−1) were analyzed in relation to a generalized rate law for mineral dissolution (Jt/m0 = k′(m/m0)γ, where Jt is the rate of dissolution and/or reduction at time t, m0 is the initial mass of oxide, and m/m0 is the unreduced or undissolved mineral fraction) in order to evaluate changes in the apparent reactivity of Fe(III) oxides during long-term biological vs. chemical reduction. The natural Fe(III) oxide assemblages demonstrated larger changes in reactivity (higher γ values in the generalized rate law) compared to the synthetic oxides during long-term abiotic reductive dissolution. No such relationship was evident in the bacterial reduction experiments, in which temporal changes in the apparent reactivity of the natural and synthetic oxides were far greater (5-10 fold higher γ values) than in the abiotic reduction experiments. Kinetic and thermodynamic considerations indicated that neither the abundance of electron donor (lactate) nor the accumulation of aqueous end-products of oxide reduction (Fe(II), acetate, dissolved inorganic carbon) are likely to have posed significant limitations on the long-term kinetics of oxide reduction. Rather, accumulation of biogenic Fe(II) on residual oxide surfaces appeared to play a dominant role in governing the long-term kinetics of bacterial crystalline Fe(III) oxide reduction. The experimental findings together with numerical simulations support a conceptual model of bacterial Fe(III) oxide reduction kinetics that differs fundamentally from established models of abiotic Fe(III) oxide reductive dissolution, and indicate that information on Fe(III) oxide reactivity gained through abiotic reductive dissolution techniques cannot be used to predict long-term patterns of reactivity toward enzymatic reduction at circumneutral pH.  相似文献   

9.
Cementitious materials used for radioactive waste repository construction complicate the performance assessment of radioactive waste systems because the use of cement may greatly alter the pH (8–13) of groundwater and release constituents such as calcium ions. Under such conditions, it is important to clarify also the dynamic behavior of silica (silicic acid), in order to evaluate the alteration in the chemical and physical properties of the fractured layer or the host rock surrounding the repository. Since silica undergoes polymerization, precipitation or dissolution depending on the pH and/or temperature, the behavior of silica would be greatly complicated in the presence of other ions. This study is focused on the deposition rates of polysilicic acid and soluble silicic acid with up to 10−3 M Ca ions. In the experiment, Na2SiO3 solution (250 mL, pH > 10, 298 K) was poured into a polyethylene vessel containing amorphous silica powder (0.5 g), and a buffer solution, HNO3, and CaNO3 as Ca ions were sequentially added into the vessel. The pH of the solution was set to 8. The silica, initially in a soluble form at pH > 10 (1.4 × 10−2 M), became supersaturated and either deposited on the solid surface or changed into the polymeric form. Then the concentrations of both poly- and soluble silicic acid were monitored over a 40-day period. The decrease of polysilicic acid became slow with an increase in the concentration of Ca ions in the range of up to 10−3 M. In general, the addition of electrolytes to a supersaturated solution accelerates the aggregation and precipitation of polymeric species. However, the experimental result showed that polysilicic acid in the presence of Ca ions is apparently stable in solution, compared with that under a Ca-free condition. On the other hand, the concentration of soluble silicic acid in the presence of Ca ions immediately became metastable, that is, slightly higher than the solubility of soluble silicic acid. Its dynamic behavior was similar to that in the Ca-free condition.  相似文献   

10.
This article represents the second of two articles, which review the main results of the international radioecological projects: Chernobyl Pilot Site Project (1999–2003) and Experimental Platform in Chernobyl (2004–2008). These projects studied radionuclide migration from the near-surface radioactive waste trench at the Red Forest waste dump in the Chernobyl zone, which contained nuclear fuel particles. This article presents results from the comprehensive hydrogeological site characterization program including the following issues: geological structure of the study site, hydraulic properties of the deposits, tracer tests in the aquifer, results of groundwater monitoring and unsaturated zone regime studies, as well as data on the 90Sr distribution in the unsaturated zone and aquifer, and analyses of 90Sr sorption behavior. The derived parameters were used to develop and calibrate 1D (flow tube) and 2D (cross-section) models describing the migration of 90Sr from the studied waste trench to the unsaturated zone and aquifer over a 16-a period (1986–2002). The models involved the following sub-models: (1) the geostatistical (structural) model for radioactivity distribution in the trench (using GSLIB); and (2) the radionuclide source term model (STERM1D) describing dissolution of fuel particles and a 1D of radionuclide redistribution in the trench body and unsaturated zone. The MODFLOW – MT3D codes were used to model the 2D 90Sr transport in the aquifer cross-section. Calibration of the 1D model with respect to Kds and dispersivities allowed quite accurate reproduction of 90Sr migration behavior for the early period (1995–1998). The less perfect fit between the 1D and 2D modeling results and monitoring data for the later period (1999–2002) suggests the need to improve the conceptual radionuclide migration model (i.e. to account for transient hydraulic and geochemical regimes of the waste site).  相似文献   

11.
Iron and Mn oxides and associated radionuclides in soils and sediments from the radioactive waste burial grounds at Oak Ridge National Laboratory have been selectively extracted using wet chemical techniques. Product-moment-correlation analyses have demonstrated that 60Co and various actinides, principally 244Cm, 241Am and 238Pu are dominantly associated with Mn oxides. Correlation coefficients between these radionuclides and Fe oxides and organic C are generally very low. The important role of Mn oxides in radionuclide adsorption is attributed to their unique surface and colloidal properties. The data illustrate the importance of the Mn oxide component of soils and sediments in controlling transition metal and actinide solubility.These results suggest two major implications for the disposal of radioactive waste. First, in order to minimize future 60Co and actinide mobilization from disposal sites, a chemical environment in which Mn oxides are least soluble should be maintained. Second, the liberal use of Mn oxides in waste management operations might improve long-term retention of these radionuclides. Deep-sea Mn modules, which may in the future be mined for their trace metal contents, could serve as a ready supply of Mn oxide for waste disposal applications.  相似文献   

12.
High-precision measurements of the oxygen isotopic compositions of carbonates (calcite and dolomite) from five CM2 chondrites are presented and put into context of the previously determined mineralogic alteration index (MAI), which places these meteorites into an alteration sequence. The carbonate oxygen isotopic compositions range from +20.0 to +35.7‰ for δ18O, +8.0 to +17.7‰ for δ17O, and −0.7 to −2.7‰ for Δ17O. Carbonate Δ17O values are inversely correlated with MAI and track the evolution of fluid composition from higher to lower Δ17O values with increasing alteration on the CM parent body. Similar Δ17O values for calcite and dolomite fractions from the same splits of the same meteorites indicate that calcite and dolomite in each split precipitated from a single fluid reservoir. However, reversed calcite dolomite fractionations (δ18Odol − δ18Occ) indicate that the fluid was subject to processes, such as freeze-thaw or evaporation, that fractionated isotopes in a mass-dependent way. Consideration of the carbonate isotopic data in the context of previously proposed models for aqueous alteration of carbonaceous chondrites has provided important insights into both the evolving alteration conditions and the utility of the models themselves. The data as a whole indicate that the isotopic evolution of the fluid was similar to that predicted by the closed-system, two-reservoir models, but that a slightly larger matrix-water fractionation factor may apply. In the context of this model, more altered samples largely reflect greater reaction progress and thus probably indicate more extended times of fluid exposure. Petrographic observations of carbonates reveal a trend of variable carbonate morphology correlated with alteration that is also consistent with changes in the duration of fluid-rock interaction. The data can also be reconciled with fluid-flow models in a restricted region of the parent body, which is consistent with assertions that the different types of carbonaceous chondrites derive from different regions of their parent bodies. In this case, the model results for a 9-km-radius body, and our data place the location of the CM chondrite formation in a 100-m-thick zone 1 km from the surface. The size of this zone could be increased if the model parameters were adjusted.  相似文献   

13.
Initial 129I/127I values (I-Xe ages) have been obtained for individual mineralogically characterized chondrules and interchondrule matrix from the enstatite chondrites Qingzhen (EH3) and Kota Kota (EH3). In view of the absence of aqueous alteration and the low-peak metamorphic temperatures experienced by these meteorites, we suggest that the I-Xe ages for the chondrules record the event in which they were formed. These ages are within the range recorded for chondrules from ordinary chondrites, demonstrating that chondrules formed during the same time interval in the source regions of both ordinary chondrites and enstatite chondrites. The timing of this chondrule-forming episode or episodes brackets the I-Xe closure age of planetesimal bodies such as the Shallowater aubrite parent body. Although chondrule formation need not have occurred close to planetesimals, the existence of planetesimals at the same time as chondrule formation provides constraints on models of this process. Whichever mechanisms are proposed to form and transport chondrules, they must be compatible with models of the protosolar nebula which predict the formation of differentiated bodies on the same timescale at the same heliocentric distance.  相似文献   

14.
In the context of a research and development program on waste disposal, an experimental site (Tournemire tunnel, Aveyron, France) was selected by the French Institute for Nuclear Protection and Safety (IPSN) in order to undertake studies on potential fluid flow at different scales of space and time within a 250-m-thick argillaceous formation. The argillite has a low natural water content (~3–5%) and very low radii access porosity. Diffusion (tritiated water) coefficients (1×10–12 to 2×10–11 m2/s) and hydraulic conductivities derived from different types of laboratory tests (10–14 to 10–13 m/s) are characteristics of a very low-permeable rock. In situ hydraulic tests (including long-term hydraulic-head measurements) were used to obtain values for hydraulic head and hydraulic conductivity at a scale of 1–10 m (10–13 to 10–11 m/s). Despite uncertainties on these data (due to a scale factor, presence of fissures, and possible artefacts due to hydro-chemo-mechanical coupling), it is expected that fluid flow is essentially governed by diffusion processes. Identification of possible natural flows at larger scales of time and space was investigated using natural isotopic tracers from interstitial fluids. Modelling, based on the deuterium profile along the clay formation and assuming pure diffusion processes, provides estimations of possible flow times. However, lack of knowledge concerning the past geological evolution of the site and the possible role of a fracture network do not permit reduction of uncertainties on these estimations at this stage. Electronic Publication  相似文献   

15.
A comparative tectonic quiescence and lack of earthquakes make the stable centres of continents attractive for siting long-term radioactive waste storage facilities. The low rates of deformation in such regions, however, make it difficult to characterize their long-term seismotectonic behaviour, leading to uncertain estimates for the very low probability hazard estimates required by society. In an attempt to overcome the deficiency of both contemporary seismicity and paleoseismic data in central Canada, we have used earthquake histories from regions with similar seismotectonic characteristics from around the world. Substituting space for time, we estimate a long-term rate per 106 km2 of 0.004 magnitude ≥6 earthquakes per annum, of which 33–100% might rupture to the surface.  相似文献   

16.
《Applied Geochemistry》2002,17(6):709-734
Uranium, Th and Pb isotopes were analyzed in layers of opal and chalcedony from individual mm- to cm-thick calcite and silica coatings at Yucca Mountain, Nevada, USA, a site that is being evaluated for a potential high-level nuclear waste repository. These calcite and silica coatings on fractures and in lithophysal cavities in Miocene-age tuffs in the unsaturated zone (UZ) precipitated from descending water and record a long history of percolation through the UZ. Opal and chalcedony have high concentrations of U (10 to 780 ppm) and low concentrations of common Pb as indicated by large values of 206Pb/204Pb (up to 53,806), thus making them suitable for U-Pb age determinations. Interpretations of U-Pb isotope systems in opal samples at Yucca Mountain are complicated by the incorporation of excess 234U at the time of mineral formation, resulting in reverse discordance of U-Pb ages. However, the 207Pb/235U ages are much less affected by deviation from initial secular equilibrium and provide reliable ages of most silica deposits between 0.6 and 9.8 Ma. For chalcedony subsamples showing normal age discordance, these ages may represent minimum times of deposition. Typically, 207Pb/235U ages are consistent with the microstratigraphy in the mineral coating samples, such that the youngest ages are for subsamples from outer layers, intermediate ages are from inner layers, and oldest ages are from innermost layers. 234U and 230Th in most silica layers deeper in the coatings are in secular equilibrium with 238U, which is consistent with their old age and closed system behavior during the past ∼0.5 Ma. The ages for subsamples of silica layers from different microstratigraphic positions in individual calcite and silica coating samples collected from lithophysal cavities in the welded part of the Topopah Spring Tuff yield slow long-term average growth rates of 1 to 5 mm/Ma. These data imply that the deeper parts of the UZ at Yucca Mountain maintained long-term hydrologic stability over the past 10 Ma. despite significant climate variations. U-Pb ages for subsamples of silica layers from different microstratigraphic positions in individual calcite and silica coating samples collected from fractures in the shallower part of the UZ (welded part of the overlying Tiva Canyon Tuff) indicate larger long-term average growth rates up to 23 mm/Ma and an absence of recently deposited materials (ages of outermost layers are 3–5 Ma.). These differences between the characteristics of the coatings for samples from the shallower and deeper parts of the UZ may indicate that the nonwelded tuffs (PTn), located between the welded parts of the Tiva Canyon and Topopah Spring Tuffs, play an important role in moderating UZ flow.  相似文献   

17.
Total concentrations of and binding capacities for Cd, Cu, and Pb were measured in selected surface waters from northwestern Europe. Linear multiple regression predictive models explained 97, 93, and 96% of the observed variation in Cd, Cu and Pb binding capacities, respectively. The models constructed used (CO23?) and (SO22?) to predict Cd binding capacity, (OH?) and (SO42?) to predict Cu binding capacity and (OH?), (CO32?) and (SO42?) to predict Pb binding capacity. Organic carbon was not significantly correlated with binding capacities for Cd, Cu, and Pb and was unimportant in explaining a significant amount of the variability in binding capacities for the metals of northern European surface waters. Thus, the effects of these organics on trace metal speciation can be ignored and predictive models of trace metal speciation constructed, using inorganic solubility equilibria only. Ratios of total Cd, Cu, and Pb concentrations to their respective binding capacities were much less than unity for all waters studied. Copper exhibited the greatest metal concentrations: binding capacity ratio in all waters investigated.  相似文献   

18.
O, Sr and C isotopes from east‐central Vermont are used to provide information on the timing and volume of metamorphic fluid flow. The results are then used to assess the evidence for redox transformations between C species. Oxygen profiles are homogenised on a metre scale; comparison with Sr isotopes suggest that O alteration may have occurred over a significantly larger timescale than that of Sr, possibly because O was modified during dewatering and diagenesis in addition to the high temperature alteration recorded by strontium. Sr isotope distributions are consistent with cross‐layer fluid fluxes of 104?106 moles m?2; absolute values depend on the Sr fluid‐rock distribution coefficient which is poorly known; however, reaction progress constraints suggest that fluxes were towards the lower end of this range. High δ13C values observed at lithological boundaries cannot be explained by volume loss or closed system processes and are taken to indicate reductive precipitation of graphite as a result of mixing between CO2 and CH4‐bearing fluids. Mass balance calculations indicate that redox reactions occurring under metamorphic conditions convert a minimum of 10% of the CO2 released from limestones into graphite, thus providing a potentially important control on the average residence time of C within the crust with implications for C cycling models.  相似文献   

19.
In this article, we model the volcanism near the proposed nuclear waste repository at Yucca Mountain, Nevada, U.S.A. by estimating the instantaneous recurrence rate using a nonhomogeneous Poisson process with Weibull intensity and by using a homogeneous Poisson process to predict future eruptions. We then quantify the probability that any single eruption is disruptive in terms of a (prior) probability distribution, since not every eruption would result in disruption of the repository. Bayesian analysis is performed to evaluate the volcanic risk. Based on the Quaternary data, a 90% confidence interval for the instantaneous recurrence rate near the Yucca Mountain site is (1.85×10–6/yr, 1.26×10–5/yr). Also, using-these confidence bounds, the corresponding 90% confidence interval for the risk (probability of at least one disruptive eruption) for an isolation time of 104 years is (1.0×10–3, 6.7×10–3), if it is assumed that the intensity remains constant during the projected time frame.  相似文献   

20.
Radioactive core samples containing elevated concentrations of Cr from a high level nuclear waste plume in the Hanford vadose zone were studied to asses the future mobility of Cr. Cr(VI) is an important subsurface contaminant at the Hanford Site. The plume originated in 1969 by leakage of self-boiling supernate from a tank containing REDOX process waste. The supernate contained high concentrations of alkali (NaOH ≈ 5.25 mol/L), salt (NaNO3/NaNO2 >10 mol/L), aluminate [Al(OH)4− = 3.36 mol/L], Cr(VI) (0.413 mol/L), and 137Cs+ (6.51 × 10−5 mol/L). Water and acid extraction of the oxidized subsurface sediments indicated that a significant portion of the total Cr was associated with the solid phase. Mineralogic analyses, Cr valence speciation measurements by X-ray adsorption near edge structure (XANES) spectroscopy, and small column leaching studies were performed to identify the chemical retardation mechanism and leachability of Cr. While X-ray diffraction detected little mineralogic change to the sediments from waste reaction, scanning electron microscopy (SEM) showed that mineral particles within 5 m of the point of tank failure were coated with secondary, sodium aluminosilicate precipitates. The density of these precipitates decreased with distance from the source (e.g., beyond 10 m). The XANES and column studies demonstrated the reduction of 29-75% of the total Cr to insoluble Cr(III), and the apparent precipitation of up to 43% of the Cr(VI) as an unidentified, non-leachable phase. Both Cr(VI) reduction and Cr(VI) precipitation were greater in sediments closer to the leak source where significant mineral alteration was noted by SEM. These and other observations imply that basic mineral hydrolysis driven by large concentrations of OH− in the waste stream liberated Fe(II) from the otherwise oxidizing sediments that served as a reductant for CrO42−. The coarse-textured Hanford sediments contain silt-sized mineral phases (biotite, clinochlore, magnetite, and ilmenite) that are sources of Fe(II). Other dissolution products (e.g., Ba2+) or Al(OH)4− present in the waste stream may have induced Cr(VI) precipitation as pH moderated through mineral reaction. The results demonstrate that a minimum of 42% of the total Cr inventory in all of the samples was immobilized as Cr(III) and Cr(VI) precipitates that are unlikely to dissolve and migrate to groundwater under the low recharge conditions of the Hanford vadose zone.  相似文献   

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