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Preliminary 3-D site-scale studies of radioactive colloid transport in the unsaturated zone at Yucca Mountain, Nevada.

The U.S. Department of Energy (DOE) is actively investigating the technical feasibility of permanent disposal of high-level nuclear waste in a repository to be situated in the unsaturated zone (UZ) at Yucca Mountain (YM), Nevada. In this study we investigate, by means of numerical simulation, the transport of radioactive colloids under ambient conditions from the potential repository horizon to the water table. The site hydrology and the effects of the spatial distribution of hydraulic and transport properties in the Yucca Mountain subsurface are considered. The study of migration and retardation of colloids accounts for the complex processes in the unsaturated zone of Yucca Mountain, and includes advection, diffusion, hydrodynamic dispersion, kinetic colloid filtration, colloid straining, and radioactive decay. The results of the study indicate that the most important factors affecting colloid transport are the subsurface geology and site hydrology, i.e., the presence of faults (they dominate and control transport), fractures (the main migration pathways), and the relative distribution of zeolitic and vitric tuffs. The transport of colloids is strongly influenced by their size (as it affects diffusion into the matrix, straining at hydrogeologic unit interfaces, and transport velocity) and by the parameters of the kinetic-filtration model used for the simulations. Arrival times at the water table decrease with an increasing colloid size because of smaller diffusion, increased straining, and higher transport velocities. The importance of diffusion as a retardation mechanism increases with a decreasing colloid size, but appears to be minimal in large colloids.

Colloids↗

Organic carbon flow in the Ob, Yenisey Rivers and Kara Sea of the Arctic region.

Stable carbon isotope and elemental C/N ratios of the organic fraction of a set of samples along a transect in the Ob and Yenisey Rivers into the Kara Sea in the Arctic were measured. Previously, the concentrations of 239,240Pu and 137Cs in these same samples had been determined. The coupled measurements were carried out to assess possible connectivity between organic carbon flow into the Kara Sea and transport of radioactive nuclides in this marine environment. Organic carbon flow into the Kara Sea is influenced significantly by terrigenous sources carried by the Ob and Yenisey Rivers. The carbon isotope-organic carbon relationship provides evidence that a rich source of terrigenous carbon exists in the riverine system. A weak, but significant relationship between stable carbon isotope ratio and 137Cs suggests that most of the 137Cs is derived from riverine particles, as compared to Pu which is also derived from in situ scavenging within the water column.

Arctic Regions↗

Modeling the potential radionuclide transport by the Ob and Yenisey Rivers to the Kara Sea.

A major portion of the former Soviet Union (FSU) nuclear program is located in the West Siberian Basin. Among the many nuclear facilities are three production reactors and the spent nuclear fuel reprocessing sites, Mayak, Tomsk-7, and Krasnoyarsk-26, which together are probably responsible for the majority of the radioactive contamination found in the Ob and Yenisey River systems that feed into the Arctic Ocean through the Kara Sea. This manuscript describes ongoing research to estimate radionuclide fluxes to the Kara Sea from these river systems. Our approach is to apply a hierarchy of simple models that use existing and forthcoming data to quantify the transport and fate of radionuclide contaminants via various environmental pathways. We present an initial quantification of the contaminant inventory, hydrology, meteorology, and sedimentology of the Ob River system and preliminary conclusions from portions of the Ob River model.

Arctic Regions↗

Beverages: bottled water. Direct final rule.

The Food and Drug Administration (FDA) is amending its bottled water quality standard regulations by establishing an allowable level for the contaminant uranium. As a consequence, bottled water manufacturers are required to monitor their finished bottled water products for uranium at least once each year under the current good manufacturing practice (CGMP) regulations for bottled water. Bottled water manufacturers are also required to monitor their source water for uranium as often as necessary, but at least once every 4 years unless they meet the criteria for the source water monitoring exemptions under the CGMP regulations. FDA will retain the existing allowable levels for combined radium-226/-228, gross alpha particle radioactivity, and beta particle and photon radioactivity. This direct final rule will ensure that the minimum quality of bottled water, as affected by uranium, combined radium-226/-228, gross alpha particle radioactivity, and beta particle and photon radioactivity, remains comparable with the quality of public drinking water that meets the Environmental Protection Agency's (EPA's) standards. FDA is issuing a direct final rule for this action because the agency expects that there will be no significant adverse comment on this rule. Elsewhere in this issue of the Federal Register, FDA is publishing a companion proposed, rule under the agency's usual procedure for notice-and-comment rulemaking, to provide a procedural framework to finalize the rule in the event the agency receives any significant adverse comments and withdraws this direct final rule. The companion proposed rule and direct final rule are substantively identical.

Consumer Product Safety↗

129I from the nuclear reprocessing facilities traced in precipitation and runoff in northern Europe.

A huge amount of radioactive 129I has been released into the environment from the nuclear energy industry, atomic weapon tests, and nuclear accidents. In this study, we present weekly and seasonal data on 129I measured in precipitation and runoff of northern Europe during 1998 and 1999. The 129I concentration is at 10(8)-10(9) atoms/L in precipitation and (2-5) x 10(8) atoms/L in runoff water, and it is 3-4 orders of magnitude higher than in the prenuclear era. Snow shows lower 129I concentration than rain, and there is apparently a positive correlation between surface air temperature and 129I. Precipitation chemistry, expressed as the content of Cl, SO4, and NO3 and atmospheric ozone, exhibits weak negative correlation with 129I values. Our 129I data on precipitation suggest significant influence of the northern European atmosphere by the discharges from the nuclear reprocessing facilities at Sellafield and La Hague.

Europe↗

Marine radioactivity assessment of Mururoa and Fangataufa atolls.

The International Atomic Energy Agency (IAEA) carried out an international project. 'The Study of the Radiological Situation at the Atolls of Mururoa and Fangataufa' with the aim of assessing the present and future radiological situation at the atolls and making recommendations for either monitoring or remedial actions if they are deemed necessary. The paper concentrates on marine radioactivity aspects and gives an estimation of present radionuclide concentrations in water, sediment and biota of the Mururoa and Fangataufa lagoons and the surrounding ocean. The dominant radionuclide in both lagoons is Pu in sediments (the total inventory is approximately 30 TBq). A decline in radionuclide concentrations has been observed in recent years in lagoon water, with the exception of 3H and 90Sr, for which a contribution from underground sources is to be expected. Radionuclide concentrations in biota from the lagoons and the surrounding ocean are low and consistent with previous measurements. The observed radionuclide concentrations in both lagoons imply that no radiological risk exists for hypothetical inhabitants of Mururoa and Fangataufa Atolls.

Animals↗

Radioactivity concentration in liquid and solid phases of scale and sludge generated in the petroleum industry.

Scales and sludge generated during oil extraction and production can contain uranium, thorium, radium and other natural radionuclides, which can cause exposure of maintenance personnel. This work shows how the oil content can influence the results of measurements of radionuclide concentration in scale and sludge. Samples were taken from a PETROBRAS unit in Northeast Brazil. They were collected directly from the inner surface of water pipes or from barrels stored in the waste storage area of the E&P unit. The oil was separated from the solids with a Soxhlet extractor by using aguarras at 90+/-5 degrees C as solvent. Concentrations of 226Ra and 228Ra in the samples were determined before and after oil extraction by using an HPGe gamma spectrometric system. The results showed an increase in the radionuclide concentration in the solid (dry) phase, indicating that the above radionuclides concentrate mostly in the solid material.

Background Radiation↗

Radon concentrations in groundwater in Busan measured with a liquid scintillation counter method.

In this paper, we present the first measurement of radon concentrations in drinking groundwater from private and public deep-bored wells located in the south-eastern area of Korea. The measurements were carried out on 439 samples by using a liquid scintillation method. The results show that the radon concentrations of the samples range from 0 to about 300 Bq l(-1). We find that Sasang ward shows the highest median value of radon concentration among 13 different wards, while Jung ward has the lowest. We find that the radon concentrations are highly dependent on the type of geological rock aquifers.

Environmental Monitoring↗

Potential for rapid transport of contaminants from the Kara Sea.

Export of sea ice from the Kara Sea may redistribute contaminants entrained from atmospheric, marine and riverine sources. Ice exiting the Kara Sea ice to the north, will influence the Fram Strait, Svalbard and Barents Sea regions. Kara Sea ice may also be exported to the Barents Sea through straits north and south of Novaya Zemlya. Some ice from the Kara Sea makes its way into the Laptev Sea to the north and south of Severnaya Zemlya. Data on ice exchange and contaminant levels are not adequate to assess contaminant flux.

Arctic Regions↗

The outflow of radionuclides from Novaya Zemlya bays--modeling and monitoring strategies.

Hydrodynamic model results are used to evaluate possible monitoring strategies for a continuous survey of underwater dump sites. The Hamburg Shelf Ocean Model (HAMSOM) is applied to Abrosimov Bay and forced with realistic, transient wind fields and air temperatures. The three-dimensional circulation model is coupled to a dynamic-thermodynamic ice model that accounts for surface heat fluxes, fractional ice cover and ice thickness. Model results show significant variations in the bay circulation due to a pronounced seasonality in the wind forcing and the ice cover. The circulation is weakest in early summer when wind speeds are low and the ice still covers most parts of the bay. In autumn, circulation and flushing of the bay is most enhanced, due to increasing wind speeds and the absence of an ice cover. Dispersion scenarios were carried out assuming a leakage at dumped objects. During most of the year the obtained tracer concentrations in the bay are higher in the upper layers than close to the bottom, indicating an outflow at the surface and a compensatory inflow below. This general pattern is only reversed during spring and early summer, when the wind directions change. Since ice problems make it almost impossible to monitor surface waters or even the whole water column in a shallow bay, the only way to install a monitoring system, is at the bottom of the bay, as close as possible to dumped objects. Data transmission via satellite or radio could be realized from a small station located on the bay's edge.

Arctic Regions↗

Sediment deposition rates on the continental margins of the eastern Arabian Sea using 210Pb, 137Cs and 14C.

Eight gravity cores from the active eastern continental margins of the Arabian Sea were dated using 210Pbxs, 137Cs and 14C. The short-term (< or = 100 years) sedimentation rates range from 0.06 to 0.66 cm/year where as the long-term (> or = 1000 years) ones using AMS 14C on planktonic foraminifera varied from 0.004 to 0.13 cm/year. For long-term chronology (< or = 50,000 years) AMS dating of well-cleaned planktonic foraminifera is most suited.

Animals↗

UraniumVI sorption behavior on silicate mineral mixtures.

UraniumVI sorption experiments involving quartz and clinoptilolite, important mineral phases at the proposed US nuclear waste repository at Yucca Mountain, NV, were conducted to evaluate the ability of surface complexation models to predict UVI sorption onto mineral mixtures based on parameters derived from single-mineral experiments. The experiments were conducted at an initial UVI aqueous concentration of approximately 2.0 x 10(-7) mol.l-1 (0.1 mol.l-1 NaNO3 matrix) and over the pH range approximately 2.5 to approximately 9.5. The UVI solutions were reacted with either quartz or clinoptilolite only, or with mixtures of the two minerals. The experiments were carried out under atmospheric pCO2(g) conditions (in loosely capped containers) or under limited pCO2(g) (in capped containers or in a glove box). Data from sorption experiments on quartz at atmospheric pCO2 conditions were used to derive UVI binding constants for a diffuse-layer surface complexation model (DLM). The DLM was then used with surface area as a scaling factor to predict sorption of UVI onto clinoptilolite and clinoptilolite/quartz mixtures under both atmospheric and low pCO2 conditions. The calculations reproduced many aspects of the pH-dependent sorption behavior. If this approach can be demonstrated for natural mineral assemblages, it may be useful as a relatively simple method for improving radionuclide transport models in performance-assessment calculations.

Adsorption↗

Retardation capacity of organophilic bentonite for anionic fission products.

Sorption and diffusivity of iodide and pertechnetate (I- and TcO4-) on MX-80 bentonite with different hexadecylpyridinium (HDPy+) loadings were studied using equilibrium solutions of different ionic strengths. In HDPy(+)-modified bentonite, iodide and pertechnetate ions exhibited increasing sorption (characterized by the distribution ratio, Rd), while Cs+ and Sr2+ showed decreasing sorption with increasing organophilicity. In case of medium-loading levels, the simultaneous sorption of anions (I- and TcO4-) and cations (Cs+ and Sr2+) was observed. Sorption of ions was influenced by the composition of the electrolytes employed. It decreased gradually with increasing ionic strength of the electrolyte solutions. The experiments revealed the general tendency that the diffusivity (Da [cm2.s-1]) for iodide and pertechnetate decreases with increasing organophilicity and increases with increasing ionic strength of the equilibrium solutions, confirming the results of the sorption experiments. Additionally, some mineralogical and chemical investigations, like IR spectral analysis of the organo-bentonite samples and exchange behavior of HDPy+, were performed. On the basis of these analyses, it was concluded that the alkylammonium ions are sorbed as (1) HDPy+ cations, (2) HDPyCl molecules and (3) micelles with decreasing binding intensities in this order.

Adsorption↗

Numerical modeling of humic colloid borne americium (III) migration in column experiments using the transport/speciation code K1D and the KICAM model.

The humic colloid borne Am(III) transport was investigated in column experiments for Gorleben groundwater/sand systems. It was found that the interaction of Am with humic colloids is kinetically controlled, which strongly influences the migration behavior of Am(III). These kinetic effects have to be taken into account for transport/speciation modeling. The kinetically controlled availability model (KICAM) was developed to describe actinide sorption and transport in laboratory batch and column experiments. Application of the KICAM requires a chemical transport/speciation code, which simultaneously models both kinetically controlled processes and equilibrium reactions. Therefore, the code K1D was developed as a flexible research code that allows the inclusion of kinetic data in addition to transport features and chemical equilibrium. This paper presents the verification of K1D and its application to model column experiments investigating unimpeded humic colloid borne Am migration. Parmeters for reactive transport simulations were determined for a Gorleben groundwater system of high humic colloid concentration (GoHy 2227). A single set of parameters was used to model a series of column experiments. Model results correspond well to experimental data for the unretarded humic borne Am breakthrough.

Americium↗

Selective removal of plutonium 238 from a canal sediment using a carbonate-chelant soil washing technology (ACT*DE*CON).

The Mound laboratory site in Miamisburg, OH, a former plutonium processing facility, contains approximately 40000 yd(3) (30,580 m3) of plutonium- and thorium-contaminated soils and sediments at levels that require remediation. Existing applicable remediation technologies are unsatisfactory, because they are expensive and do not provide volume reduction. ACT*DE*CON is a chemical soil leaching technology for the treatment of soils that utilizes contaminant dissolution via dilute selective solutions to remove radionuclides. In bench-scale tests, process parameters were developed for the optimal treatment of the Miami Erie Canal soil at the Mound site, combining the maximum plutonium removal with an acceptable amount of soil dissolution and minimizing the costs of reagents. Parameters evaluated included soil to extractant mass ratio, temperature, rinse solution composition, kinetics, and the application of several dewatering aids. Plutonium removal rates of >95% were achieved, and the residual plutonium in the treated soil proved to be very immobile-confirming that the process had removed the most accessible species of the radionuclide. Currently being tested at Mound is an engineering scale-up that includes an attrition scrubber, a counter-current extractor, and a reverse osmosis system. Economic evaluations based on bench-scale results put the treatment cost at US$278/yd(3) (US$364/m3), compared to US$350/yd(3) (US$458/m3) for the 'box-and-bury' baseline alternative treatment system.

Carbonates↗

Ultrafiltration of large volumes for the determination of colloidally bound artificial radionuclides in natural waters.

A methodology based on large volume ultrafiltration (> 1000 l) is developed in order to characterize the artificial radionuclides associated with the colloidal populations in natural waters. "Inorganic elements" and organic carbon sinks or sources due to sorption or post desorption within the ultrafiltration assembly/membranes of the Sartorius system are underlined and discussed from methodological step experiments as well as recoveries obtained for artificial radionuclides such as 106Ru, 125Sb, 137Cs and 239+240Pu fractionating natural waters from the Rhône River (France), its estuary and the Mediterranean Sea (Gulf of Lions).

Colloids↗