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PubMed2003

Probabilistic assessment of contamination using the two-phase flow model.

A physically motivated model is indispensable for a successful analysis of the impact of leaching from nuclear waste storage sites on the environment and public health. While most analyses use the single-phase flow model for modelling unsaturated flow and solute transport, the two-phase flow model considering the resistance of gas to water flow is a more realistic one. The effect of the two-phase flow model on the water content is theoretically investigated first in this study. Then, by combining a geostatistical generator using the turning bands method and a multi-phase transport code TOUGH2, an automatic process is used for Monte Carlo simulation of the solute transport. This stochastic approach is applied to a potentially polluted site by low-level nuclear waste in Taiwan. In the simulation, the saturated hydraulic conductivity is treated as the random variable. The stochastic approach provides a probabilistic assessment of contamination. The results show that even though water content from the two-phase flow model is only 1.5% less than the one from the single-phase flow model, the two-phase flow causes a slower movement but a wider lateral spreading of the plume in the unsaturated zone. The stochastic approach provides useful probability information which is not available from the deterministic approach. The probability assessment of groundwater contamination provides the basis for more informed waste management, better environmental assessment and improved evaluation of impact on public health.

Forecasting↗
PubMed2003

Effect of temperature on Cs+ sorption and desorption in subsurface sediments at the Hanford Site, U.S.A.

The effects of temperature on Cs+ sorption and desorption were investigated in subsurface sediments from the U.S. Department of Energy Hanford Site. The site has been contaminated at several locations by the accidental leakage of high-level nuclear waste (HLW) containing 137Cs+. The high temperature of the self-boiling, leaked HLW fluid and the continuous decay of various radionuclides carried by the waste supernatant have resulted in elevated vadose temperatures (currently up to 72 degrees C) below the Hanford S-SX tank farm that have dissipated slowly from the time of leakage (1970). The effect of temperature on Cs+ sorption was evaluated through batch binary Cs(+)-Na+ exchange experiments on pristine sediments, while Cs+ desorption was studied in column experiments using 137Cs(+)-contaminated sediments. Cs+ adsorption generally decreased with increasing temperature, with a more apparent decrease at low aqueous Cs+ concentration (10(-10)-10(-6) mol/L). Cs+ desorption from the contaminated sediments increased with increasing temperature. The results indicated that the free energy of Na(+)-Cs+ exchange on the Hanford sediment had a significant enthalpy component that was estimated to be -17.87 (+/- 2.01) and -4.82 (+/- 0.44) kJ/mol (at 298 degrees C) for the high- and low-affinity exchange sites, respectively. Both Cs+ adsorption and desorption at elevated temperature could be well simulated by a two-site ion exchange model, with the conditional exchange constants corrected by the exchange enthalpy effect. The effect of temperature on Cs+ desorption kinetics was also evaluated using a stop-flow technique. The kinetics of desorption of the exchangeable pool (which was less than the total adsorbed concentration) were found to be rapid under the conditions studied.

Adsorption↗
PubMedDate not supplied

Effect of heterogeneity on radionuclide retardation in the alluvial aquifer near Yucca Mountain, Nevada.

The U.S. Department of Energy is currently studying Yucca Mountain, Nevada, as a potential site for a geological high-level waste repository. In the current conceptual models of radionuclide transport at Yucca Mountain, part of the transport path to pumping locations would be through an alluvial aquifer. Interactions with minerals in the alluvium are expected to retard the downstream migration of radionuclides, thereby delaying arrival times and reducing ground water concentrations. We evaluate the effectiveness of the alluvial aquifer as a transport barrier using the stochastic Lagrangian framework. A transport model is developed to account for physical and chemical heterogeneities and rate-limited mass transfer between mobile and immobile zones. The latter process is caused by small-scale heterogeneity and is thought to control the macroscopic-scale retardation in some field experiments. A geostatistical model for the spatially varying sorption parameters is developed from a site-specific database created from hydrochemical measurements and a calibrated modeling approach (Turner and Pabalan 1999). Transport of neptunium is considered as an example. The results are sensitive to the rate of transfer between mobile and immobile zones, and to spatial variability in the hydraulic conductivity. Chemical heterogeneity has only a small effect, as does correlation between hydraulic conductivity and the neptunium distribution coefficient. These results illustrate how general sensitivities can be explored with modest effort within the Lagrangian framework. Such studies complement and guide the application of more detailed numerical simulations.

Actinoid Series Elements↗
PubMed1985

Carbon-14 discharge at three light-water reactors.

A long-term-sampling evaluation was made of the quantity, discharge pathway, and chemical form of 14C released from 2 pressurized water reactors (PWR) and 1 boiling water reactor (BWR) in the northeastern United States. For the R. E. Ginna PWR the discharge rate of gaseous 14C was 11.6 Ci/GW(e)-yr. Venting of gas decay tanks accounted for 42%, while 35% was discharged through auxiliary building ventilation and 23% through containment venting. The average chemical composition was 10% as 14CO2, 90% as 14CH4 and other hydrocarbon gases. For the Indian Point Unit 3 PWR, the discharge rate was 9.6 Ci/GW(e)-yr, primarily by pressure-relief venting and purging of the containment air. Venting of gas decay tanks accounted for about 7% of the total released. The chemical species were 26% 14CO2, 74% 14CH4 and other hydrocarbon gases. For the J. A. FitzPatrick BWR, the discharge rate was 12.4 Ci/GW(e)-yr. Approximately 97% of the release was via off-gas discharge, which was about 95% 14CO2. For all 3 reactors the quantity of 14C released with liquid and solid wastes was less than 5% of the gaseous release.

Air Pollutants↗
PubMed2004

A cation exchange model to describe Cs+ sorption at high ionic strength in subsurface sediments at Hanford site, USA.

A theoretical and experimental study of cation exchange in high ionic strength electrolytes was performed using pristine subsurface sediments from the U.S. Department of Energy Hanford site. These sediments are representative of the site contaminated sediments impacted by release of high level waste (HLW) solutions containing 137Cs+ in NaNO3 brine. The binary exchange behavior of Cs+-Na+, Cs+-K+, and Na+-K+ was measured over a range in electrolyte concentration. Vanselow selectivity coefficients (Kv) that were calculated from the experimental data using Pitzer model ion activity corrections for aqueous species showed monotonic increases with increasing electrolyte concentrations. The influence of electrolyte concentration was greater on the exchange of Na+-Cs+ than K+-Cs+, an observation consistent with the differences in ion hydration energy of the exchanging cations. A previously developed two-site ion exchange model [Geochimica et Cosmochimica Acta 66 (2002) 193] was modified to include solvent (water) activity changes in the exchanger phase through application of the Gibbs-Duhem equation. This water activity-corrected model well described the ionic strength effect on binary Cs+ exchange, and was extended to the ternary exchange system of Cs+-Na+-K+ on the pristine sediment. The model was also used to predict 137Cs+ distribution between sediment and aqueous phase (Kd) beneath a leaked HLW tank in Hanfordd's S-SX tank using the analytical aqueous data from the field and the binary ion exchange coefficients for the pristine sediment. The Kd predictions closely followed the trend in the field data and were improved by consideration of water activity effects that were considerable in certain regions of the vadose zone plume.

Cations↗
PubMed2001

Reactive barriers for 137Cs retention.

137Cs was dispersed globally by cold war activities and, more recently, by the Chernobyl accident. Engineered extraction of 137Cs from soils and groundwaters is exceedingly difficult. Because the half-life of 137Cs is only 30.2 years, remediation might be more effective (and less costly) if 137Cs bioavailability could be demonstrably limited for even a few decades by use of a reactive barrier. Essentially permanent isolation must be demonstrated in those few settings where high nuclear level wastes contaminated the environment with 135Cs (half-life 2.3 x 10(6) years) in addition to 137Cs. Clays are potentially a low-cost barrier to Cs movement, though their long-term effectiveness remains untested. To identify optimal clays for Cs retention, Cs desorption was measured for five common clays: Wyoming Montmorillonite (SWy-1), Georgia Kaolinites (KGa-1 and KGa-2), Fithian Illite (F-Ill), and K-Metabentonite (K-Mbt). Exchange sites were pre-saturated with 0.16 M CsCl for 14 days and readily exchangeable Cs was removed by a series of LiNO3 and LiCl washes. Washed clays were then placed into dialysis bags and the Cs release to the deionized water outside the bags measured. Release rates from 75 to 139 days for SWy-1, K-Mbt and F-Ill were similar; 0.017% to 0.021% sorbed Cs released per day. Both kaolinites released Cs more rapidly (0.12% to 0.05% of the sorbed Cs per day). In a second set of experiments, clays were Cs-doped for 110 days and subjected to an extreme and prolonged rinsing process. All the clays exhibited some capacity for irreversible Cs uptake. However, the residual loading was greatest on K-Mbt (approximately 0.33 wt.% Cs). Thus, this clay would be the optimal material for constructing artifical reactive barriers.

Adsorption↗
PubMed1996

Radionuclides in fishes and mussels from the Farallon Islands Nuclear Waste Dump Site, California.

The Farallon Islands Nuclear Waste Dump Site (FINWDS), approximately 30 miles west of San Francisco, California, received at least 500 TBq encapsulated in more than 47,500 containers from approximately 1945 to 1970. During several seasons in 1986/87 deep-sea bottom feeding fishes (Dover sole = Microstomus pacificus; sablefish = Anoplopoma fimbria; thornyheads = Sebastolobus spp.) and intertidal mussels (Mytilus californianus) were collected from the vicinity of the FINWDS and from comparable depths at a reference site near Point Arena, CA. Tissues were analyzed for several radionuclides (137Cs, 238Pu, 239+240Pu, and 241Am). Radionuclide concentrations for fish mussel tissue ranged from non-detectable to 4,340 mBq kg(-1) wet weight, with the following means for Farallon fishes: 137Cs = 1,110 mBq kg(-1); 238Pu = 390 mBq kg(-1); 239+240Pu = 130 mBq kg(-1); and 241Am = 1,350 mBq kg(-1). There were no statistically significant differences in the radionuclide concentrations observed in samples from the Farallon Islands compared to reference samples from Point Arena, CA. Concentrations of both 238Pu and 241Am in fish tissues (from both sites) were notably higher than those reported in literature from any other sites world-wide, including potentially contaminated sites. Concentrations of 239+24OPu from both sites were typical of low values found at some contaminated sites worldwide. These results show approximately 10 times higher concentrations of 239+240Pu and approximately 40-50 times higher concentrations of 238Pu than those values reported for identical fish species from 1977 collections at the FINWDS. Radionuclide concentrations were converted to a hypothetical per capita annual radionuclide intake for adults, yielding the following values of annual Committed Effective Dose Equivalent (CEDE) from ionizing radiation emitted from these radionuclides: 0.000 mSv y(-1) for 137Cs, 0.009 mSv Y(-1) for 228Pu, and 0.003 mSv y(-1) for 239+240Pu. For 241Am, projected CEDE for Dover sole, sablefish, and thornyheads were higher, averaging 0.03 mSv y(-1). The observed isotopic ratio of 238Pu/239+240Pu was about 4 (which is two orders of magnitude higher than the ratio of 0.03 associated with fallout from weapons tests and accidental releases in the north temperate zone of the earth), indicating a considerably higher environmental mobilization for 238Pu compared to 239+240Pu. Likewise, the observed ratio of 241Am/239+240Pu of about 30 was nearly two orders of magnitude higher than the fallout ratio of 0.43 in the north temperate zone of the earth. The projected ionizing radiation CEDE to people from the ingestion of fish with fallout radionuclides was three times higher for 241Am than from the plutonium isotopes.

Alpha Particles↗
PubMed2001

Cover design for radioactive and AMD-producing mine waste in the Ronneburg area, eastern Thuringia.

At the former uranium mining site of Ronneburg, large scale underground and open pit mining for nearly 40 years resulted in a production of about 113,000 tonnes of uranium and about 200 million cubic metres of mine waste. In their present state, these materials cause risks to human health and strong environmental impacts and therefore demand remedial action. The remediation options available are relocation of mine spoil into the open pit and on site remediation by landscaping/contouring, placement of a cover and revegetation. A suitable vegetated cover system combined with a surface water drainage system provides long-term stability against erosion and reduces acid generation thereby meeting the main remediation objectives which are long-term reduction of radiological exposure and contaminant emissions and recultivation. The design of the cover system includes the evaluation of geotechnical, radiological, hydrological, geochemical and ecological criteria and models. The optimized overall model for the cover system has to comply with general conditions as, e.g. economic efficiency, public acceptance and sustainability. Most critical elements for the long-term performance of the cover system designed for the Beerwalde dump are the barrier system and its long-term integrity and a largely self-sustainable vegetation.

Environmental Monitoring↗
PubMed2004

Identification of the non-pertechnetate species in Hanford waste tanks, Tc(I)--carbonyl complexes.

Immobilization of the high-level nuclear waste stored at the Hanford Reservation has been complicated by the presence of soluble, lower-valent technetium species. Previous work by Schroeder and Blanchard has shown that these species cannot be removed by ion-exchange and are difficult to oxidize. The Tc K-edge XANES spectra of the species in Tanks SY-101 and SY-103 were reported by Blanchard, but they could not be assigned to any known technetium complex. We report that the XANES spectra are most likely those of Tc(I)-carbonyl species, especially fac-Tc(CO)3(gluconate)(2-). This is further supported by EXAFS and 99Tc-NMR studies in nonradioactive simulants of these tank wastes.

Carbon↗
PubMed1999

Critical radionuclide/critical pathway analysis for the U.S. Department of Energy's Savannah River Site.

Many different radionuclides have been released to the environment from the Savannah River Site (SRS) during the facility's operational history. However, as shown by this analysis, only a small number of the released radionuclides have been significant contributors to potential doses and risks to off-site people. This article documents the radiological critical contaminant/critical pathway analysis performed for SRS. If site missions and operations remain constant over the next 30 years, only tritium oxide releases are projected to exceed a maximally exposed individual (MEI) risk of 1.0E-06 for either the airborne or liquid pathways. The critical exposure pathways associated with site airborne releases are inhalation and vegetation consumption, whereas the critical exposure pathways associated with liquid releases are drinking water and fish consumption. For the SRS-specific, nontypical exposure pathways (i.e., recreational fishing and deer and hog hunting), cesium-137 is the critical radionuclide.

Air Pollutants, Radioactive↗
PubMed2000

Stabilization and solidification of metal-laden wastes by compaction and magnesium phosphate-based binder.

Bench-scale and full-scale investigations of waste stabilization and volume reduction were conducted using spiked soil and ash wastes containing heavy metals such as Cd, Cr, Pb, Ni, and Hg. The waste streams were stabilized and solidified using chemically bonded phosphate ceramic (CBPC) binder, and then compacted by either uniaxial or harmonic press for volume reduction. The physical properties of the final waste forms were determined by measuring volume reduction, density, porosity, and compressive strength. The leachability of heavy metals in the final waste forms was determined by a toxicity characteristic leaching procedure (TCLP) test and a 90-day immersion test (ANS 16.1). The structural composition and nature of waste forms were determined by X-ray diffraction (XRD) and scanning electron microscopy (SEM), respectively. CBPC binder and compaction can achieve 80-wt% waste loading and 39-47% reduction in waste volume. Compressive strength of final waste forms ranged from 1500 to 2000 psi. TCLP testing of waste forms showed that all heavy metals except Hg passed the TCLP limits using the phosphate-based binder. When Na2S was added to the binder, the waste forms also passed TCLP limits for Hg. Long-term leachability resistance of the final waste forms was achieved for all metals in both soil and ash wastes, and the leachability index was approximately 14. XRD patterns of waste forms indicated vermiculite in the ash waste was chemically incorporated into the CBPC matrix. SEM showed that waste forms are layered when compacted by uniaxial press and are homogeneous when compacted by harmonic press.

Hazardous Waste↗
PubMed1985

Compliance and policy issues and recommendations related to revision of the National Interim Primary Drinking Water Regulations for Radionuclides.

This paper summarizes the deliberations and conclusions of the Compliance and Policy Committee of the National Workshop for Radioactivity in Drinking Water. Prior to and during the workshop the committee considered a total of 32 possible compliance and policy issues and determined that 22 were valid. The committee developed positions on seven of these and these positions are presented herein. The remaining 25 issues are also listed with the committee's evaluation of each.

Legislation as Topic↗
PubMed1999

Tritium and plutonium in waters from the Bering and Chukchi seas.

During the summer of 1993, seawater in the Bering and Chukchi Seas was sampled on a joint Russian-American cruise [BERPAC] of the RV Okean to determine concentrations of tritium, 239Pu and 240Pu. Concentrations of tritium were determined by electrolytic enrichment and liquid scintillation counting. Tritium levels ranged up to 420 mBq L(-1) and showed no evidence of inputs other than those attributed to atmospheric nuclear weapons testing. Plutonium was recovered from water samples by ferric hydroxide precipitation, and concentrations were determined by thermal ionization mass spectrometry. 239+240Pu concentrations ranged from < 1 to 5.5 microBq L(-1). These concentrations are lower than those measured in water samples from other parts of the ocean during the mid-1960's to the late 1980's. The 240Pu:239Pu ratios, although associated with large uncertainties, suggest that most of the plutonium is derived from world-wide fallout. As points of comparison, the highest concentrations of tritium and plutonium observed here were about five orders of magnitude lower than the maximum permissible concentrations allowed in water released to the off-site environs from licensed nuclear facilities in the United States. This study and others sponsored by the International Atomic Energy Agency and the Office of Naval Research's Arctic Nuclear Waste Assessment Program are providing data for the assessment of potential radiological impacts in the Arctic regions associated with nuclear waste disposal by the former Soviet Union.

Oceans and Seas↗