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PubMedDate not supplied

The measurement of technetium-99 and iodine-129 in waste water from pressurized nuclear-power reactors.

The program for measuring the dispersal presence of contaminating nuclides in waste streams produced by pressurized-water-reactor (PWR) power plants required the establishment of analytical procedures for a number of nuclides. In this report the procedure to assess 99Tc and 129I content in liquid samples using liquid-scintillation counting is presented. 99Tc and 129I are adsorbed on AG 1 X2 ion-exchange resin. 129I is then eluted with NaOCl and further purified by liquid-liquid extraction using carbon tetrachloride and an aqueous solution of sodium thiosulphate. 99Tc is eluted with hot nitric acid (6 M/60 degrees C). If necessary any 60Co present in the sample is separated by liquid-liquid extraction of the cobalt-TTA complex with iso-BuOH. The overall recovery yield is 96.5 +/- 2.5% for 99Tc and 90.1 +/- 6.2% for 129I. Finally beta-activity is measured by liquid-scintillation counting. A limit of detection of 5 Bq/L can thus be obtained for both 99Tc and 129I.

Belgium↗

PubMed2003

Diffusivity measurement of heavy ions in Wyoming montmorillonite gels by X-ray computed tomography.

Medical X-ray computed tomography (CT) was applied to the measurement of the diffusion coefficients of heavy ions in an artificial barrier material for the disposal of nuclear wastes. Cs(+), Sr(2+), I(-), and Br(-) are the heavy ions measured and the barrier used is the water-rich gel of Wyoming montmorillonite (86.5-100 wt.% H(2)O). X-ray CT yields an inevitable artifact (beam-hardening) in the obtained images. Before the diffusion experiments, the polychromatic primary X-ray spectrum of the CT scanner was measured by a CdZnTe detector, and the effects of the artifact were examined for an aqueous CsCl solution sample. The results show that the beam-hardening artifact derived from the polychromatic photon energy distribution can be suppressed by applying a special image reconstruction method assuming the chemical composition of samples. The transient one-dimensional diffusion of heavy ions in a plastic container filled with the gel was imaged nondestructively by the X-ray CT scanner with an in-plane resolution of 0.31 mm and slice thickness of 2 mm. The results show that diffusivities decrease with increasing clay weight fraction. The degree of the diffusivity decrease was high for cations (Cs(+) and Sr(2+)) and low for anions (I(-) and Br(-)). The quantitative decomposition of the contribution of the geometrical tortuosity and of the sorption to the diffusivity was performed by subtracting the diffusivity of nonsorbing I(-) from the measured diffusivities. The results show that the contribution of the sorption is large for Cs(+), Sr(2+) and small for Br(-). Because X-ray CT allows nondestructive and quick measurements of diffusivities, the technique would be useful particularly for measuring the diffusive migration of harmful radioactive elements.

Bentonite↗

PubMed1997

Microbial studies in the Canadian nuclear fuel waste management program.

Atomic Energy of Canada Limited (AECL) has developed a concept for permanent geological disposal of used nuclear fuel in Canada. This concept, based on a multibarrier system, would involve disposal of nuclear fuel waste in titanium or copper containers, surrounded by compacted clay-based buffer and backfill materials, in a vault 500-1000 m deep in granitic rock of the Canadian Shield. Subsurface environments will not be sterile and an experimental program was initiated in 1991 by AECL to address and quantify the potential effects of microbial action on the integrity of the disposal vault. This microbial program focuses on answering specific questions in areas such as the survival of bacteria in compacted clay-based buffer materials under relevant radiation, temperature and desiccation conditions; mobility of microbes in compacted buffer materials; the potential for microbially influenced corrosion of containers; microbial gas production in backfill material; introduction of nutrients as a result of vault excavation and operation; the presence and activity of microbes in deep granitic groundwaters; and the effects of biofilms on radionuclide migration in the geosphere. This paper summarizes the results to date from the research activities at AECL.

Bacterial Physiological Phenomena↗

PubMed2002

Products of pertechnetate radiolysis in highly alkaline solution: structure of TcO2 x xH2O.

The chemistry of technetium in certain high-level nuclear waste (HLW) tanks at the Hanford Site complicates the treatment and vitrification of HLW. A major problem is the presence, in certain tanks, of unidentified, lower-valent technetium species, which are difficult to remove from the waste by current separation processes. Radiolytic reduction of TcO4- in alkaline solutions containing selected organic compounds, approximating the conditions in HLW, was investigated to determine the classes of compounds that can be formed under these conditions. Insoluble TcO2 x xH2O is the primary radiolysis product with the majority of organic compounds investigated, including citrate, dibutyl phosphate, and aminopolycarboxylates. X-ray absorption fine structure (XAFS) measurements show that TcO2 x xH2O has a one-dimensional chain structure consisting of edge-sharing TcO6 octahedra with bridging oxide and trans water ligands. When diols, such as ethylene glycol, are present, only soluble, Tc(IV) alkoxide compounds are produced. The XAFS and UV-visible spectra of these compounds provide evidence for a binuclear structure similar to (H2EDTA)2Tc2(mu-O)2. The properties of the Tc(IV) alkoxide complexes were determined and are consistent with those observed for the soluble, lower-valent technetium complexes that complicate the treatment of HLW at the Hanford site.

Oxygen↗

PubMed1991

Perceived risk, stigma, and potential economic impacts of a high-level nuclear waste repository in Nevada.

This study investigates the potential impacts of the proposed nuclear waste repository at Yucca Mountain, Nevada, upon tourism, retirement and job-related migration, and business development in Las Vegas and the state. Adverse impacts may be expected to result from perceptions of risk, stigmatization, and socially amplified reactions to "unfortunate events" associated with the repository (major and minor accidents, discoveries of radiation releases, evidence of mismanagement, attempts to sabotage or disrupt the facility, etc.). The conceptual underpinnings of risk perception, stigmatization, and social amplification are discussed and empirical data are presented to demonstrate how nuclear images associated with Las Vegas and the State of Nevada might trigger adverse economic effects. The possibility that intense negative imagery associated with the repository may cause significant harm to Nevada's economy can no longer be ignored by serious attempts to assess the risks and impacts of this unique facility. The behavioral processes described here appear relevant as well to the social impact assessment of any proposed facility that produces, uses, transports, or disposes of hazardous materials.

Humans↗

PubMed1987

An analysis of the portfolio of sites to characterize for selecting a nuclear repository.

The U.S. Department of Energy has selected three sites, from five nominated, to characterize for a nuclear repository to permanently dispose of nuclear waste. This decision was made without the benefit of an analysis of this "portfolio" problem. This paper analyzes different portfolios of three sites for simultaneous characterization and strategies for sequential characterization. Characterization of each site, which involves significant subsurface excavation, is now estimated to cost $1 billion. Mainly because of the high characterization costs, sequential characterization strategies are identified which are the equivalent of $1.7-2.0 billion less expensive than the selected DOE simultaneous characterization of the three sites. If three sites are simultaneously characterized, one portfolio is estimated to be the equivalent of $100-400 million better than the selected DOE portfolio. Because of these potential savings and several other complicating factors that may influence the relative desirability of characterization strategies, a thorough analysis of characterization strategies that addresses the likelihood of finding disqualifying conditions during site characterization, uncertainties, and dependencies in forecast site repository costs, preclosure and postclosure health and safety impacts, potential delays of both sequential and simultaneous characterization strategies, and the environmental, socioeconomic, and health and safety impacts of characterization activities is recommended.

Radioactive Waste↗

PubMed2003

Occupational health services at ten U.S. Department of Energy weapons sites.

BACKGROUND: Nuclear weapons sites are among thousands of federal facilities that are contaminated with a variety of hazardous wastes. Workers at these sites participate in a wide array of activities that can result in their exposure to a variety of hazards. METHODS: The purpose of this study was to describe the occupational health and safety services at ten U.S. Department of Energy sites. Interviews were conducted with 30 health and safety professionals, including physicians, program managers, and industrial hygienists. Data collection was guided by a quality assessment model that provided a means to examine the structures, processes, and outcomes of occupational health and safety services. RESULTS: It was determined that services for some worker groups, such as subcontractors, were limited; other problems identified included a mismatch between hazards (physical hazards) and types of service providers (radiation experts), ineffective databases, and communication problems. CONCLUSIONS: This description of health and safety services has provided valuable information that can be used to improve the efficiency and effectiveness of service delivery in this large and complex organization.

Communication↗

PubMed1997

Behavior of Na131I and meta(131I) iodobenzylguanidine (MIBG) in municipal sewerage.

Behavior of 131I activity in primary sludge at the Ann Arbor, Michigan, Municipal Waste Water Treatment Plant was studied in relation to known radioiodine therapy events at the University of Michigan Hospital complex. The principal compounds administered are Na131I, which has widespread use, and meta (131I) iodobenzylguanidine (MIBG), which is a compound unique to the University of Michigan, although labeled antibodies and other forms are also used in therapy and research. The objectives of the study were to determine the environmental fate of such discharges and to determine radiation exposures to workers and the public when sludges are incinerated. Approximately 17% of the MIBG activity administered in a therapy was found in the primary sludge, whereas only 1.1% of the Na131I was in sludge. When land applied, the short half life of 131I in the sludge presents few radiological health concerns; however, incineration, which is done in winter months, is assumed to release organically bound 131I to the atmosphere. Radiation doses due to incineration of sludge containing measured concentrations were calculated for a maximally exposed worker to be 1.7 microSv (0.17 mrem) of which 0.48 microSv (0.048 mrem) was due to a 2-d upset condition. For a more typically exposed worker, and a member of the public, the committed effective dose equivalents were 1.2 microSv (0.12 mrem) and 0.06 microSv (0.006 mrem), respectively, for a 22-wk incineration period with release of all radioiodine in the sludge. Transport time to the treatment plant for radioiodine was found to be much longer than that of normal sewage, possibly due to organic material in sewer lines that absorb iodine. The residence time of radioiodine in the sewer also appears to be longer than expected; whether other radioactive materials are held up the same way is not known but chemical form is surely a factor.

3-Iodobenzylguanidine↗

PubMedDate not supplied

Seepage into drifts with mechanical degradation.

Seepage into drifts in unsaturated tuff is an important issue for the long-term performance of the proposed nuclear waste repository at Yucca Mountain, Nevada. Drifts in which waste packages will be emplaced are subject to degradation in the form of rockfall from the drift ceiling, induced by stress-relief, seismic, or thermal effects. The objective of this study is to calculate seepage rates, for various drift-degradation scenarios and for different values of percolation flux, in the Topopah Spring middle nonlithophysal (Tptpmn) and the Topopah Spring lower lithophysal (Tptpll) units at Yucca Mountain. Seepage calculations are conducted by (1) defining a heterogeneous drift-scale permeability model with field data, (2) selecting calibrated parameters associated with the Tptpmn and Tptpll units, and (3) simulating seepage, based on detailed degraded-drift profiles obtained from a separate rock mechanics engineering analysis. The simulation results indicate (1) that the seepage threshold (i.e., the percolation flux at which seepage first occurs) is not significantly changed by drift degradation and (2) the degradation-induced increase in seepage above the threshold is influenced probably more by the shape of the cavity created by rockfall than by rockfall volume.

Geological Phenomena↗

PubMed2002

Population mixing and leukaemia in young people around the La Hague nuclear waste reprocessing plant.

In order to investigate for an association between population mixing and the occurrence of leukaemia in young people (less than 25 years), a geographical study was conducted, for the years 1979 to 1998, in Nord Cotentin (France). This area experienced between the years 1978 and 1992 a major influx of workers for the construction of a nuclear power station and a new nuclear waste reprocessing unit. A population mixing index was defined on the basis of the number of workers born outside the French department of 'La Manche' and living in each 'commune', the basic geographical unit under study. The analyses were done with indirect standardisation and Poisson regression model allowing or not for extra-Poisson variation. Urban 'communes' were considered as the reference population. The Incidence Rate Ratio was 2.7 in rural 'communes' belonging to the highest tertile of population mixing (95% Bayesian credible interval, 95%BCI=1.2-5.9). A positive trend was observed among rural strata with increasing population mixing index (IRR for trend=1.4, 95%BCI=1.1-1.8). The risk became stronger for Acute Lymphoblastic Leukaemia in children 1-6 years old in the highest tertile of population mixing (IRR=5.5, 95%BCI=1.4-23.3). These findings provide further support for a possible infective basis of childhood leukaemia.

Adolescent↗

PubMed2003

Geochemical modelling of bentonite porewater in high-level waste repositories.

The description of the geochemical properties of the bentonite backfill that serves as engineered barrier for nuclear repositories is a central issue for performance assessment since these play a large role in determining the fate of contaminants released from the waste. In this study the porewater chemistry of bentonite was assessed with a thermodynamic modelling approach that includes ion exchange, surface complexation and mineral equilibrium reactions. The focus was to identify the geochemical reactions controlling the major ion chemistry and acid-base properties and to explore parameter uncertainties specifically at high compaction degrees. First, the adequacy of the approach was tested with two distinct surface complexation models by describing recent experimental data performed at highly varying solid/liquid ratios and ionic strengths. The results indicate adequate prediction of the entire experimental data set. Second, the modelling was extended to repository conditions, taking as an example the current Swiss concept for high-level waste where the compacted bentonite backfill is surrounded by argillaceous rock. The main reactions controlling major ion chemistry were found to be calcite equilibrium and concurrent Na-Ca exchange reactions and de-protonation of functional surface groups. Third, a sensitivity analysis of the main model parameters was performed. The results thereof indicate a remarkable robustness of the model with regard to parameter uncertainties. The bentonite system is characterised by a large acid-base buffering capacity which leads to stable pH-conditions. The uncertainty in pH was found to be mainly induced by the pCO(2) of the surrounding host rock. The results of a simple diffusion-reaction model indicate only minor changes of porewater composition with time, which is primarily due to the geochemical similarities of the bentonite and the argillaceous host rock. Overall, the results show the usefulness of simple thermodynamic models to describe porewater chemistry of expandable clays although significant uncertainties with regard to the effects of swelling and physico-chemical properties of the interstitial water remain.

Bentonite↗

PubMed2005

Uncertainty in rate loss corrections based on counting a periodic pulser.

Tomographic gamma scanning of waste produces three-dimensional transmission and emission images. These are used to derive item-specific attenuation correction factors that improve the accuracy of non-destructive waste assay. For each vertical layer, data grabs of short duration are acquired as the waste item is rotated and translated. The image reconstruction demands accurate rate loss corrections to minimize assay bias. For this application a pulser was used to perform the necessary rate loss corrections. In this work, we summarize the benefits of the pulser approach and review the basic principles on which the method is based. We extend the treatment to include a derivation of the expression for the uncertainty in the net pulser peak area in the presence of an underlying continuum. We report experimental results, taken using a Canberra model WM2900 Tomographic Gamma Scanner, over a broad range of count-rates and peak-to-continuum ratios. Repeat counts under controlled conditions allowed the correction factor and its variance to be determined and compared against expectations. These results confirm the validity of the correction factor formula and the corresponding expression for its uncertainty. The rate loss analysis has been built into a Monte Carlo Replicate engine to allow the uncertainty to be propagated into the total measurement uncertainty of the final assay.

Gamma Rays↗

PubMed1997

Microbiology in nuclear waste disposal: interfaces and reaction fronts.

It is now generally acknowledged that microbial populations will be present within nuclear waste repositories and that the consequences of such activity on repository performance must be assessed. Various modelling approaches--based either on mass balance/thermodynamics or on kinetics--have been developed to provide scoping estimates of the possible development of these populations. Past work has focused on particular areas of the repository which can be considered relatively homogeneous and hence can be represented by some kind of 'box' or 'mixing tank'. In reality, however, waste repositories include a range of engineering materials (steel, concrete, etc.) which are emplaced at depth in a rock formation. Strong chemical gradients--of the type which may be exploited by lithoautotrophic microbial populations--are likely to be found at the contacts between different materials and at the interface between the engineered structures and the host rock. Over the long timescales considered, solute transport processes will cause the locations of strong chemical gradients to move, forming reaction fronts. The high-pH plume resulting from the leaching of cement/concrete in some repository types is a particularly important example of such a reaction front. Redox fronts, which may occur in different areas of all kinds of repositories, also play an important role and would be locations where microbial activity is likely to be significant. In this paper, the key microbial processes expected at (or around) interfaces and fronts will be discussed, with particular emphasis on the development of quantitative models. The applicability of the models used wil be tested by considering similar fronts which can be found in natural systems.

Biodegradation, Environmental↗

PubMed2001

Nitrate-cancrinite precipitation on quartz sand in simulated Hanford tank solutions.

Caustic NaNO3 solutions containing dissolved Al were reacted with quartz sand at 89 degrees C to simulate possible reactions between leaked nuclear waste and primary subsurface minerals at the U.S. Department of Energy's Hanford site in Washington. Nitrate-cancrinite began to precipitate onto the quartz after 2-10 days, cementing the grains together. Estimates of the equilibrium constant for the precipitation reaction differ for solutions with 0.1 or 1.0 m OH- (log Keq = 30.4 +/- 0.8 and 36.2 +/- 0.6, respectively). The difference in solubility may be attributable to more perfect crystallinity (i.e., fewer stacking faults) in the higher-pH cancrinite structure. This is supported by electron micrographs of crystal morphology and measured rates of Na volatilization under an electron beam. Precipitate crystallinity may affect radionuclide mobility, because stacking faults in the cancrinite structure can diminish its zeolitic cation exchange properties. The precipitation rate near the onset of nucleation depends on the total Al and Si concentrations in solution. The evolution of experimental Si concentrations was modeled by considering the dependence of quartz dissolution rate on AI(OH)4- activity, cancrinite precipitation, and the reduction of reactive surface area of quartz due to coverage by cancrinite.

Aluminum↗

PubMed2001

What views and uses of radiation sources in the 21st century?

Considering that in 1899 neither biotechnology nor the electronic revolution were foreseen, some humility might be advisable when one looks into the crystal ball for the future role of radiation sources. In the past 50 years, nuclear medicine, nuclear weapons, and nuclear power have had a huge impact in the world. In the next 50 years, nuclear weapons may be phased out, nuclear power revived, and nuclear medicine may continue, especially for diagnostic purposes. Conflicts between great powers and blocks will no longer be about territorial or ideological domination but about trade, finance, information, and the environment and the weapons used will not be bombs but investments, credits, and control of information. Nuclear power-still based on fission-will be relaunched and get more uses, e.g., to propel ships, to produce heat for industry and for space heating, and perhaps to desalinate water. The public will be more at ease with radiation as it is better educated, as nuclear safety continuously improves and new types of nuclear power plants emerge, as waste sites fail to cause any problems, and as no other energy source is found to deliver so much energy at reasonable cost with negligible impact on climate and environment. One kilogram of oil corresponds to 4 kWh of electricity. One kilogram of uranium fuel corresponds to 50,000 kWh, and 1 kg of plutonium 6,000,000 kWh! In nuclear medicine, radiation may give way to other treatments as the understanding of cancer advances. On the other hand, the extreme ease with which sources of radiation can be identified is unmatched and likely to make them useful tools as tracers and markers in medicine-and other fields-for a long time. For certain uses--perhaps food irradiation--radiation sources, such as cobalt, may be replaced by accelerators which may be switched on and off at will. As more sources are used, registration and control of them must be made very effective around the whole world. Very high natural emissions of radon will continue to call for cautionary measures, but many other nonradiating substances will be identified as hazardous to health and call for vigorous intervention.

Forecasting↗

PubMed2006

Numerical simulation of reactive processes in an experiment with partially saturated bentonite.

Bentonites are preferred materials for use as engineered barriers for high-level nuclear waste repositories. Simulation of geochemical processes in bentonite is therefore important for long-term safety assessment of those repositories. In this work, the porewater chemistry of a bentonite sample subject to simultaneous heating and hydration, as studied by Cuevas et al. [Cuevas, J., Villar, M., Fernández, A., Gómez, P., Martín, P., 1997. Porewaters extracted from compacted bentonite subjected to simultaneous heating and hydration. Applied Geochemistry 12, 473-481.], was assessed with a non-isothermal reactive transport model by coupling the geochemical software PHREEQC2 with the object-oriented FEM simulator GeoSys/RockFlow. Reactive transport modelling includes heat transport, two-phase flow, multicomponent transport and geochemical reactions in the liquid phase, i.e. ion exchange, mineral dissolution/precipitation and equilibrium reactions. Simulations show that the easily soluble minerals in bentonite determine the porewater chemistry. Temperature affects both two-phase flow and geochemical reactions. Porosity change due to dissolution/precipitation is low during the experiment. However, changes of the effective porosity caused by bentonite swelling can be very large. The simulated results agree well with the experimental data.

Bentonite↗

PubMed2006

Sorption of Am(III) onto 6-line-ferrihydrite and its alteration products: investigations by EXAFS.

For the long-term performance assessment of nuclear waste repositories, knowledge about the interactions of actinide ions with mineral surfaces such as iron oxides is imperative. The mobility of released radionuclides is strongly dependent on the sorption/desorption processes at these surfaces and on their incorporation into the mineral structure. In this study the interaction of Am(III) with 6-line-ferrihydrite (6LFh) was investigated by EXAFS spectroscopy. At low pH values (pH 5.5), as well at higher pH values (pH 8.0), Am(III) sorbs as a bidentate corner-sharing species onto the surface. Investigations of the interaction of Am(III) with Fh coated silica colloids prove the sorption onto the iron coating and not onto the silica substrate. Hence, the presence of Fh, even as sediment coating, is the dominant sorption surface. Upon heating, Fh is transformed into goethite and hematite as shown by TEM and IR measurements. The results of the fit to the EXAFS data indicate the release of sorbed Am(III) at pH 5.5 during the transformation and likely a partial incorporation of Am into the Fh transformation products at pH 8.0.

Americium↗

PubMed1996

Depth-dose distribution in bricks determined by thermoluminescence and by Monte-Carlo calculation for external gamma-dose reconstruction.

The analysis of depth-dose distributions in bricks sampled from walls in areas with nuclear waste or accident contamination has the potential of providing information on the energy and source configuration of the gamma-radiation that had been incident on the brick. In this study, a brick from a mill facing a shallow water reservoir of the contaminated Techa river in the South Ural region is investigated. Thermoluminescence (TL) methods were used to measure the accumulated dose at several depths in the brick. The accidental external gamma-dose is obtained by subtracting the natural radiation background dose from the total accumulated dose. In the first segment of the brick, at a depth of about 1.5 cm, the accident dose was found to be roughly 3.5 Gy. Monte-Carlo simulations of the photon transport from the reservoir bed contaminated with 137Cs were calculated for different depths in the brick. The calculations were made assuming different attenuating water levels. It is found that the depth-dose distribution determined by measurements corresponds to a water level between 20 and 50 cm. The results indicate that TL measurements combined with Monte-Carlo modelling calculations are highly promising for external gamma-dose reconstruction applications.

Beta Particles↗