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Description: We present a quantitative model to describe transport of radionuclides underground. Applicable to unsaturated (vadose) as well as saturated (phreatic) layers, the model provides constraints on the in-situ migratory behavior of radioisotopes in dissolved and colloidal pools of a groundwater system. It shows, for examples, that uranium in water percolating through the vadose zone will have its concentration and ratio {sup 234}U/{sup 238}U linearly correlated under the ideal condition of a constant removal of the two U isotopes from vadose-zone solids. The intercept and slope of the linearity serve to constrain removal rates of the two uranium isotopes from solids to the solution through dissolution and alpha recoil. The model also allows estimation of the fluid transit time in the vadose zone. At Pena Blanca, the uneven distribution of rainfall between winter (wet) and summer (dry) results in a conspicuous seasonal variability in uranium removal rate, hence dissolved uranium signals, within the unsaturated zone. Our data indicate a much higher uranium dissolution rate during the dry season than during the wet season, possibly reflecting a condition of increased oxygenation in the zone during the dry period.
Date: July 1, 2005
Creator: Ku, T.L.; Luo, S.; Murrell, M. & Goldstein, S.
Partner: UNT Libraries Government Documents Department

Characterization of contaminant transport using naturally-occurring U-series disequilibria. 1998 annual progress report

Description: 'The goal of the research is to study the migratory behavior of contaminants in subsurface fractured systems using naturally occurring uranium- and thorium-series radionuclides as tracers under in-situ physico-chemical and hydrogeologic conditions. Naturally occurring U- and Th-series disequilibria can provide information on the rates of adsorption-desorption and transport of contaminants as well as on fluid transport and rock dissolution in a natural setting. The authors are developing a realistic model of contaminant migration in the Snake River Plain Aquifer beneath the INEEL by evaluating the retardation processes involved in the rock/water interaction. The major tasks are to: (1) determine the natural distribution of U, Th, Pa and Ra isotopes in the groundwater as well as in rock minerals and sorbed phases, and (2) study rock/water interaction processes using U/Th series disequilibria and a statistical analysis-based model code for the calculation of in-situ retardation factors of radionuclides and rock/water interaction time scales. This study will also provide an improved understanding of the hydrogeologic features of the site and their impact on the migration of contaminants. This report summarizes results after 20 months of a 36-month project. Studies performed at LANL include analysis of the long-lived nuclides {sup 238}U, {sup 235}U, {sup 234}U, {sup 230}Th, {sup 226}Ra, {sup 232}Th, and {sup 231}Pa by thermal ionization mass spectrometry (TIMS). Studies performed at the Univ. of Southern California include the measurement of short-lived naturally occurring radionuclides by decay-counting techniques and the development of models to predict the migration behavior of these radionuclides. Initial efforts began with analysis of 31, 0.5L water samples obtained through routine sampling by USGS and INEEL personnel. One significant observation from these data is that {sup 234}U/{sup 238}U activity ratios are highest in waters that emanate from local recharge areas to the northwest of the INEEL and they decrease in ...
Date: June 1, 1998
Creator: Murrell, M. & Ku, T.L.
Partner: UNT Libraries Government Documents Department

Characterization of calculation of in-situ retardation factors of contaminant transport using naturally-radionuclides and rock/water interaction occurring U-Series disequilibria timescales. 1997 annual progress report

Description: 'The research is directed toward a quantitative assessment of contaminant transport rates in fracture-rock systems using uranium-series radionuclides. Naturally occurring uranium-and thorium-series radioactive disequilibria will provide information on the rates of adsorption-desorption and transport of radioactive contaminants as well as on fluid transport and rock dissolution in a natural setting. This study will also provide an improved characterization of preferential flow and contaminant transport at the Idaho Environmental and Engineering Lab. (INEEL) site. To a lesser extent, the study will include rocks in the unsaturated zone. The authors will produce a realistic model of radionuclide migration under unsaturated and saturated field conditions at the INEEL site, taking into account the retardation processes involved in the rock/water interaction. The major tasks are to (1) determine the natural distribution of U, Th, Pa and Ra isotopes in rock minerals. sorbed phases on the rocks, and in fluids from both saturated and unsaturated zones at the site, and (2) study rock/water interaction processes using U/Th series disequilibrium and a statistical analysis-based model for the Geologic heterogeneity plays an important role in transporting contaminants in fractured rocks. Preferential flow paths in the fractured rocks act as a major pathway for transport of radioactive contaminants in groundwaters. The weathering/dissolution of rock by groundwater also influences contaminant mobility. Thus, it is important to understand the hydrogeologic features of the site and their impact on the migration of radioactive contaminants. In this regard, quantification of the rock weathering/dissolution rate and fluid residence time from the observed decay-series disequilibria will be valuable. By mapping the spatial distribution of the residence time of groundwater in fractured rocks, the subsurface preferential flow paths (with high rock permeability and short fluid residence time) can be determined.'
Date: October 30, 1997
Creator: Roback, R.; Murrel, M.; Goldstein, S.; Ku, T.L. & Luo, S.
Partner: UNT Libraries Government Documents Department

Modeled tephra ages from lake sediments, base of Redoubt Volcano, Alaska

Description: A 5.6-m-long lake sediment core from Bear Lake, Alaska, located 22 km southeast of Redoubt Volcano, contains 67 tephra layers deposited over the last 8750 cal yr, comprising 15% of the total thickness of recovered sediment. Using 12 AMS {sup 14}C ages, along with the {sup 137}Cs and {sup 210}Pb activities of recent sediment, we evaluated different models to determine the age-depth relation of sediment, and to determine the age of each tephra deposit. The age model is based on a cubic smooth spline function that was passed through the adjusted tephra-free depth of each dated layer. The estimated age uncertainty of the 67 tephras averages {+-} 105 yr (1{sigma}). Tephra-fall frequency at Bear Lake was among the highest during the past 500 yr, with eight tephras deposited compared to an average of 3.7 per 500 yr over the last 8500 yr. Other periods of increased tephra fall occurred 2500-3500, 4500-5000, and 7000-7500 cal yr. Our record suggests that Bear Lake experienced extended periods (1000-2000 yr) of increased tephra fall separated by shorter periods (500-1000 yr) of apparent quiescence. The Bear Lake sediment core affords the most comprehensive tephrochronology from the base of the Redoubt Volcano to date, with an average tephra-fall frequency of once every 130 yr.
Date: February 25, 2007
Creator: Schiff, C J; Kaufman, D S; Wallace, K L; Werner, A; Ku, T L & Brown, T A
Partner: UNT Libraries Government Documents Department


Description: For nuclear waste management, an important mechanism by which radioactive waste components are isolated from returning to the human environment, the biosphere, is by the geological barrier in which the effectiveness of the barrier is characterized by in-situ retardation factor, i.e., the transport rate of a radionuclide relative to that of groundwater. As part of natural analog studies of the Yucca Mountain Project of the U. S. Department of Energy, we propose such characterization by using naturally-occurring decay-series radioisotopes as an analog. We collected large-volume (>1000 liters) groundwater samples from three wells (PB, Pozos, and PB4, respectively) near the Nopal I Uranium Ore site at Pena Blanca, Mexico, by using an in-situ Mn-cartridge filtration technique for analysis of short-lived decay-series radionuclides. Results show that the activities of short-lived radioisotopes ({sup 228}Ra, {sup 224}Ra and {sup 223}Ra) and activity ratios of {sup 224}Ra/{sup 228}Ra and {sup 224}Ra/{sup 223}Ra are higher at PB and Pozos than at PB4. In contrast, the {sup 210}Po activity is much lower at PB and Pozos than at PB4. The high Ra activities and activities ratios at PB and Pozos are attributable to the high alpha-recoil input from the aquifer rocks, while the high {sup 210}Po activity at PB4 is due to the enhanced colloidal transport. Based on a uranium-series transport model, we estimate that the in-situ retardation factor of Ra is (0.43 {+-} 0.02) x 10{sup 3} at PB, (1.68 {+-} 0.08) x 10{sup 3} at Pozos, and (1.19 {+-} 0.08) x 10{sup 3} at PB4 and that the mean fracture width in the aquifer rocks is about 0.23 {micro}m at PB, 0.37 {micro}m at Posos, and 4.0 {micro}m at PB4, respectively. The large fracture width at PB4 as derived from the model provides an additional evidence to the inference from the Po measurements that particle-reactive ...
Date: July 11, 2005
Creator: Luo, S.; Ku, T.L.; Todd, V.; Murrell, M.; Pineda, J. Alfredo Rodriguez; Dinsmoor, J. et al.
Partner: UNT Libraries Government Documents Department

Modeling non-steady state radioisotope transport in the vadose zone--A case study using uranium isotopes at Pena Blanca, Mexico

Description: Current models using U- and Th-series disequilibria to study radioisotope transport in groundwater systems mostly consider a steady-state situation. These models have limited applicability to the vadose zone (UZ) where the concentration and migratory behavior of radioisotopes in fluid are often transitory. We present here, as a first attempt of its kind, a model simulating the non-steady state, intermittent fluid transport in vadose layers. It provides quantitative constraints on in-situ migration of dissolved and colloidal radioisotopes in terms of retardation factor and rock-water interaction (or water transit) time. For uranium, the simulation predicts that intermittent flushing in the UZ leads to a linear relationship between reciprocal U concentration and {sup 234}U/{sup 238}U ratio in percolating waters, with the intercept and slope bearing information on the rates of dissolution and {alpha}-recoil of U isotopes, respectively. The general validity of the model appears to be borne out by the measurement of uranium isotopes in UZ waters collected at various times over a period during 1995-2006 from a site in the Pena Blanca mining district, Mexico, where the Nopal I uranium deposit is located. Enhanced {sup 234}U/{sup 238}U ratios in vadose-zone waters resulting from lengthened non-flushing time as prescribed by the model provide an interpretative basis for using {sup 234}U/{sup 238}U in cave calcites to reconstruct the regional changes in hydrology and climate. We also provide a theoretical account of the model's potential applications using radium isotopes.
Date: June 1, 2009
Creator: Ku, T. L.; Luo, S.; Goldstein, S. J.; Murrell, M. T.; Chu, W. L. & Dobson, P. F.
Partner: UNT Libraries Government Documents Department

Pena Blanca Natural Analogue Project: Summary of activities

Description: The inactive Nopal I uranium mine in silicic tuff north of Chihuahua City, Chihuahua, Mexico, was studied as a natural analogue for an underground nuclear-waste repository in the unsaturated zone. Site stratigraphy was confirmed from new drill cores. Data from site studies include chemical and isotopic compositions of saturated- and unsaturated-zone waters. A partial geochronology of uranium enrichment and mineralization was established. Evidence pertinent to uranium-series transport in the soil zone and changing redox conditions was collected. The investigations contributed to preliminary, scoping-level performance assessment modeling.
Date: February 1, 2011
Creator: Levy, S.; Goldstein, S.; Dobson, P.F.; Goodell, P.; Ku, T.-L.; Abdel-Fattah, A. et al.
Partner: UNT Libraries Government Documents Department