Nuclear Waste Storage Investigations Project Research Articles

Actinide behavior on crushed rock columns

The interactions of dissolved or colloidal actinides with tuffaceous rock are being studied at Los Alamos National Laboratory in support of the Nevada Nuclear Waste Storage Investigations project. We have used small columns of crushed tuff to obtain information on the sorption of neptunium, plutonium and americium during short (<1 day) time spans. Data from these experiments supplement information obtained from longer term batch-type experiments and provide insight concerning sorption kinetics, speciation, and colloid migration. We find that Np(V), Pu(VI) and Pu(V) show limited sorption on crushed tuff. Pu(IV) polymer and Am(III) are largely retained by the tuff, with a small fraction of the imput material moving through the column as colloids.

Elevated temperature (hydrothermal) stability of cementitious sealants for a deep geological repository in tuff

Grout formulations have been investigated in Nevada Nuclear Waste Storage Investigations Project, for possible nuclear waste repository sealing applications focused in the Yucca Mountain Area (in welded tuff). A shrinkage compensated cement was chemically modified with siliceous reactants to enhance the chemical compatibility with a siliceous tuff. Fluids in contact with the grouts were measured at 150 °C and 200 °C, and the solids were characterized. Well-crystallized Al-substituted tobermorite and truscottite were observed, and sometimes xonotlite as dominant cementitious phases. Comparisons of solid phases and solution phases are made with a second grout incorporating siliceous modifiers in a Class H cement. Exposures to 150 °C hydrothermal conditions have not produced significant detrimental mechanical behavior of the seal material. The thermal decomposition of ettringite, an expansive calcium sulfate aluminate hydrate, resulted in a small increase in the porosity of the grout, but on a very small fine scale.

Monitoring the Vadose Zone in Fractured Tuff

Unsaturated tuff beneath Yucca Mountain, Nevada, is being evaluated by the U.S. Department of Energy as a host rock for a potential repository for high-level radioactive waste. As part of the Nevada Nuclear Waste Storage Investigations Project of the U.S. Department of Energy, the U.S. Geological Survey has been conducting hydrologic, geologic and geophysical investigations at Yucca Mountain and the surrounding region to provide data for evaluation of the potential suitability of the site. Hydrologic investigations of the unsaturated zone at this site began in 1982. A 17.5-inch- (44.5-centimeter) diameter borehole (USW UZ-1) was drilled by the reverse-air vacuum-drilling technique to a depth of 1269 feet (387 meters). This borehole was instrumented at 33 depth levels. At 15 of the levels, three well screens were embedded in coarse-sand columns. The sand columns were isolated from each other by thin layers of bentonite, columns of silica flour, and isolation plugs consisting of expansive cement. Thermocouple psychrometers and pressure transducers were installed within the screens and connected to the data-acquisition system at the land surface through thermocouple and logging cables. Two of the screens at each level were equipped with access tubes to allow collection of pore-gas samples. In addition to these instruments, 18 heat-dissipation probes were installed within the columns of silica flour, some of which also had thermocouple psychrometers. After more than two years of monitoring, the majority of the instruments were still functioning and producing reasonable data. A slow recovery from the disturbed state to natural conditions was detected during the first 90 days of monitoring; this recovery was probably a result of the large diameter of the borehole. Preliminary results indicated that suction pressures for the welded units ranged from −2 to −15 bars (−0.2 to −1.5 mega pascals). Some agreement existed between data from psychrometers and from heat-dissipation probes, except where silica flour was not in equilibrium with the formation. Water fluxes estimated in the matrix of the repository host-rock unit range from 4 × 10−3 to 2 × 10−2 inches per year (0.1 to 0.5 millimeter per year) using matric-potential distribution, and from −1 × 10−3 to −2 × 10−3 inches per year (−0.025 to −0.05 millimeter per year) using geothermal gradient. Responses to short-term barometric fluctuations were detected to a maximum depth of about 300 feet (91 meters) in the borehole. Below this depth, only long-term barometric fluctuations were detectable. Equivalent effective hydraulic conductivity, estimated from air permeability, ranged from 0.6 to 2 feet per day (0.2 to 0.6 meters per day).

Preliminary Geochemical/Geophysical Model of Yucca Mountain

AbstractAs part of the Nevada Nuclear Waste Storage Investigations (NNWSI) Project, a comprehensive geochemical/geophysical model is being compiled. This model incorporates the current and relevant stratigraphic, petrologic, hydrogeologic, geochemical, and material data associated with a candidate repository at Yucca Mountain, Nevada. In this report the known repository data are compiled and unknown parameter values are estimated based on the available data. More data are needed before the geochemical/geophysical model of Yucca Mountain can be regarded as satisfactory and a suitable base for multidimensional predictive flow and transport simulations. Recommendations for future studies concerning site characterization and data aquisition are presented.

Impact of Phase Stability on the Corrosion Behavior of the Austenitic Candidate Materials For NNSWI.

AbstractThe Nuclear Waste Management Program at Lawrence Livermore National Laboratory is responsible for the development of the waste package design to meet the Nuclear Regulatory Commission licensing requirements for the Nevada Nuclear Waste Storage Investigations (NNWSI) Project. The metallic container component of the waste package is required to assist in providing substantially complete containment of the waste for a period of up to 1000 years. Long term phase stability of the austenitic candidate materials (304L and 316L stainless steels and alloy 825) over this time period at moderate temperatures (100–250°C) can impact the mechanical and corrosion behavior of the metal barrier.A review of the technical literature with respect to phase stability of 304L, 316L and 825 is presented. The impact of martensitic transformations, carbide precipitation and intermediate (σ. χ, and η) phase formation on the mechanical properties and corrosion behavior of these alloys at repository relevant conditions is discussed. The effect of sensitization on intergranular stress corrosion cracking (IGSCC) of each alloy is also addressed. A summary of the impact of phase stability on the degradation of each alloy in the proposed repository environment is included.

Summary of Results From the Series 2 and Series 3 NNWSI Bare Fuel Dissolution Tests

AbstractThe Nevada Nuclear Waste Storage Investigations (NNWSI) Project is studying dissolution and radionuclide release behavior of spent nuclear fuel in Nevada Test Site groundwater. Specimens prepared from pressurized water reactor (PWR) fuel rod segments were tested for multiple cycles in J-13 well water. The Series 2 tests were run in unsealed silica vessels under ambient hot cell air (25°C) for five cycles for a total of 34 months. The Series 3 tests were run in sealed stainless steel vessels at 25°C and 85°C for three cycles for a total of 15 months. Selected summary results from Series 2 and Series 3 tests with bare fuel specimens are reported.Actinide concentrations tended to saturate and then often decreased during test cycles. Uranium concentrations in later test cycles ranged from 1 to 2 μg/ml in the Series 2 Tests versus about 0.1 to 0.4 μg/ml in Series 3 with the lowest concentrations occurring in the 85°C tests. Formation of a calciumuranium-silicate phase identified as uranophane in the 85°C Series 3 Tests is thought to have limited uranium concentration in these tests. Americium-241, Pu-239 and Pu-240 activities measured in filtered solution decreased to less than 1 pCi/ml in the 85°C tests. Preferential release of fission products Cs, I, Sr and Tc, and activation product C-14, was indicated relative to the actinides. Tc-99 and Cs-137 activities measured in solution after Cycle 1 increased linearly with time, with the rate of increase greater at 85°C than at 25°C. Continuous preferential release of soluble fission products is thought to result primarily from the dissolution of fine particles of fission product phases concentrated on grain boundaries.

The Performance Of Actinide-Containing Srl 165 Type Glass In Unsaturated Conditions

AbstractAs part of the effort by the Nevada Nuclear Waste Storage Investigations (NNWSI) Project to evaluate the volcanic tuff beds of Yucca Mountain, Nevada, as a repository for the permanent storage of high-level nuclear waste, the interaction of actinide-doped Savannah River Laboratory (SRL) 165 type glass with the unsaturated repository environment has been studied. The NNWSI Unsaturated Test method has been used, and the results from batch and continuous tests completed through 18 months demonstrate that several interactions are important for controlling both the reaction of the glass and the release of radionuclides. These interactions include (1) the reaction between the glass and moist air with interludes of liquid water contact, which results in the release of alkali metals from the glass; and (2) the reaction between standing water, glass, and presensitized 304 L type stainless steel which results in breakdown of the glass matrix and the release of radionuclides from the glass-metal assemblage. A comparison of the results of the Unsaturated Test with those of parametric experiments illustrates the importance of presensitized steel in enhancing the glass reaction, and demonstrates the applicability of the Unsaturated Test to those conditions anticipated to exist in the NNWSI repository horizon.

Saturated permeability measurements on pumice and welded-tuffaceous materials

Fluid flows in consolidated porous media of volcanic origin are being investigated to support such diverse efforts as the modeling of thermal/outgassing phenomena at Mount St. Helens and the hydrological modeling of tuffaceous rocks in support of the Department of Energy’s (DOE) Nevada Nuclear Waste Storage Investigations Project An experimental apparatus was designed and built to allow water-saturated permeabilities as low as 10−18 m2 to be measured on cores of diameter 5 cm and length 10 cm under steady-state flow conditions. This same apparatus can also be utilized in a transient (pressure-decay) mode in order to measure permeabilities several orders of magnitude lower than the steady-state limit. Tests were conducted on samples of pumice, fractured welded tuff, and welded tuff, representing a permeability range of seven orders of magnitude Pumice was found to have a permeability of ∼3×10−12 m2, sufficiently high to allow the complete Darcy-to-Ergun regime to be investigated Welded (unfractured) tuff was tested in the transient mode, yielding a permeability of ∼5×10−19 m2. Two, long-time-scale, steady-flow experiments were conducted on a core of welded tuff containing a single, through-going fracture. For the first experiment, the core was an integral cylinder containing a naturally occurring fracture. For the second experiment, the core was separated into two pieces along the existing fracture plane, then rejoined. Effects of essentially constant, as well as rapidly varied, circumferential stress were studied in both tests. Results showed core permeability to decay to 2×10−18 m2 in both cases, independent of the initial fracture state (closed versus open). With a naturally occurring fracture, core permeability decreased by a factor of 2 over a 200-h test period. With an initially open fracture, core permeability decreased by a factor of 4 under the influence of a comparable 200-h load-time history, after 700 h of testing, core permeability was reduced by an order of magnitude from its initial level. Final effective hydraulic fracture aperture was calculated to be 10−6 m, corresponding to a calculated effective fracture permeability of 10−13 m2 Fracture flow was thus estimated to account for 80% of the total flow rate through this core under final test conditions.

Analysis of the elastic and strength properties of Yucca Mountain tuff, Nevada : Price, R H; Bauer, S J In: Research and Engineering Applications in Rock Masses (paper to the 26th US Symposium on Rock Mechanics, Rapid City, 26–28 June 1985)V1, P89–96. Publ Rotterdam: A. A. Balkema, 1985

Yucca Mountain, located near the southwest margin of the Nevada Test Site, in southern Nevada, is being evaluated as a potential site for a nuclear waste repository. Yucca Mountain consists primarily of layered volcanic tuff. Samples from four stratigraphic units have been tested for physical, thermal and mechanical properties as part of the Nevada Nuclear Waste Storage Investigations (NNWSI) Project, administered by the Nevada Operations Office of the U.S. Department of Energy. The four units, in order of increasing depth, are as follows: (1) Topopah Spring Member of the Paintbrush Tuff, (2) Tuffaceous Beds of Calico Hills, (3) Bullfrog Member of the Crater Flat Tuff, and (4) Tram Member of the Crater Flat Tuff. A large data base from more than 100 experiments on drillhole core samples of Yucca Mountain silicic tuff has been assembled for use in NNWSI site evaluation and repository design calculations. These data have been analyzed and empirical expressions were found which relate elastic properties and strength with porosity plus clay content. These relationships will be presented here, in addition to an application of simple elastic composite theory to explain the observed variation of bulk modulus with functional porosity.

Zeolitization of Glassy Topopah Spring Tuff Under Hydrothermal Conditions

AbstractIn support of the Nevada Nuclear Waste Storage Investigations Project experiments were conducted to study the effects of heat generated by a nuclear waste repository in densely welded, devitrified tuff on the underlying, compositionally-equivalent glassy tuff at Yucca Mtn. Solid wafers of glassy tuff were reacted with a dilute ground water for several months at 150°C and 250°C at 100 bars pressure in Dickson-type, gold-bag rocking autoclaves. The in-situ chemistry of the hydrothermal fluids was modeled and the chemical affinities for all possible mineral precipitation reactions (contained within the extensive database) were calculated using the EQ3/6 program.In the 250°C experiment the calculations suggest that a zeolite mineral would be expected to form. Analyses of the run products showed that not only had the wafer been extensively corroded and the glass shards replaced by clinoptilolite, but pure clinoptilolite had precipitated directly from solution. In the 150°C experiment, although clay minerals were thermodynamically favored to form in the first half of the experiment, by the end of the run a zeolite mineral was predicted to form. Analyses of the run products showed no well-formed secondary minerals (clays or zeolites) had formed. At the lower temperature the effects of precipitation kinetics may preclude the formation of the zeolite within the time span of this experiment. In general the observations are in relatively good agreement with the geochemical model calculations. This type of study demonstrates the interpretive/predictive capabilities of a combined experimental/geochemical modeling approach to studies of nuclear waste isolation. This combined approach will aid in satisfying licensing requirements to assure long-term performance.

Hydrogen Speciation in Hydrated Layers on Nuclear Waste Glass

AbstractThe hydration of an outer layer on nuclear waste glasses is known to occur during leaching, but the actual speciation of hydrogen (as water or hydroxyl groups) in these layers has not been determined. As part of the Nevada Nuclear Waste Storage Investigations Project, we have used infrared spectroscopy to determine hydrogen speciations in three nuclear waste glass compositions (SRL-131 &amp; 165, and PNL 76-68), which were leached at 90°C (all glasses) or hydrated in a vapor-saturated atmosphere at 202°C (SRL-131 only). Hydroxyl groups were found in the surface layers of all the glasses. In addition, molecular water was found in the surface of SRL-131 and PNL 76-68 glasses that had been leached for several months in deionized water, and in the vapor-hydrated sample. The water/hydroxyl ratio increases with increasing reaction time; molecular water makes up most of the hydrogen in the thick reaction layers on vapor-phase hydrated glass while only hydroxyl occurs in the least reacted samples. Using the known molar absorptivities of water and hydroxyl in silica-rich glass the vapor-phase layer contained 4.8 moles/liter of molecular water, and 0.6 moles water in the form hydroxyl. A 15 micrometer layer on SRL-131 glass formed by leaching at 90°C contained a total of 4.9 moles/liter of water, 2/3 of which was as hydroxyl. The unreacted bulk glass contains about 0.018 moles/liter water, all as hydroxyl.The amount of hydrogen added to the SRL-131 glass was about 70% of the original Na + Li content, not the 300% that would result from alkali-hydronium ion (H30+) interdiffusion. If all the hydrogen is then assumed to be added as the result of alkali-H+ interdiffusion, the molecular water observed may have formed from condensation of the original hydroxyl groups according to:20H = H20 molecular + 00where 00 refers to a bridging oxygen, and OH refers to a hydroxyl group attached to a silicate polymer. The hydrated layer on the nuclear waste glasses appears to be of relatively low water content (4 to 7% by weight) and is not substantially hydroxylated. Thus, these layers do not have many of the properties associated with “gel” layers.

The Effects Of Gamma Radiation on Groundwater Chemistry and Glass Reaction In a Saturated Tuff Environment

AbstractThe Nevada Nuclear Waste Storage Investigations project has completed a series of experiments that provide insight into groundwater chemistry and glass waste form performance in the presence of a gamma radiation field at 90°C. Results from experiments done at 1 × 103 and 0 R/hr are presented and compared to similar experiments done at 2 × 105 and 1 × 104R/hr. The major effect of radiation is to lower the groundwater pH to a value near 6.4. The addition of glass to the system results in slightly more basic final pH, both in the presence and absence of radiation. However, there is essentially no difference in the extent of glass reaction, as measured by elemental release, as a function of dose rate or total dose, for reaction periods up to 278 days.

Transport and Reaction Kinetics at the Glass:Solution Interface Region: Results of Repository-Oriented Leaching Experiments

AbstractRepository-oriented leaching experiments involving Savannah River Laboratory (SRL) 165 type glass under a γ-radiation field (1= 0.2 × 104 R/h) have been performed by the Nevada Nuclear Waste Storage Investigations (NNWSI) project. In this communication, we discuss glass surface analyses obtained by SEM, nuclear resonance profiling, and SIMS together with leachate solution data in relation to a mechanism that couples diffusion, hydrolysis (etching and gelation), and precipitation to qualitatively describe the release of different glass components to the leachant solutions. The release of mobile (e.g., Li) and partly mobile (e.g., B) species is controlled primarily by interdiffusion with water species across the interdiffusion zone. Glass components that are immobile in the interdiffusion zone are released to the solution by etching. For prediction of long-term steady-state concentrations of glass components with low solubility, the relative rates of release from the glass and secondary mineral precipitation must be taken into account.

Ambient temperature testing of the G-tunnel heated block : Zimmerman, R M; Board, M P; Hardin, E L; Voegele, M D In: rock mechanics in productivity and protection (paper to the 25th symposium on rock mechanics, Evanston, Illinois, 25–27 June 1984) P281–295. Publ New York: AIME, 1984

The G-Tunnel heated block experiment is being conducted on the Nevada Test Site (NTS) as part of the Nevada Nuclear Waste Storage Investigations project (NNWSI). The purpose of the ambient temperature testing phase is to evaluate rock-mass mechanical properties of a block ({approx} m/sup 3/) under biaxial stress changes up to 7.5 MPa above an initialization in situ value of 3.1 MPa. Results indicate that the modulus of deformation ranges from 9.7 to 17.0 GPa and Poisson`s ratio ranges from 0.21 to 0.33. In general, the higher values of the modulus and Poisson`s ratio were influenced by fracture propagations parallel to the compressive stress field. Other measurements indicated that cross-hole compression (p) wave velocities and single fracture permeability values were relatively insensitive to stress changes above the in situ value.

Hydrothermal Interaction of Topopah Spring Tuff With J-13 Water as a Function of Temperature

AbstractIn support of the Nevada Nuclear Waste Storage Investigations Project experiments were conducted to study the hydrothermal interaction of rock and water representative of a potential repository in tuff. These experiments provided data relevant to near-field repository conditions that can be used to: assess the ability to use “accelerated” tests based on the SA/V (surface area/volume) parameter and temperature; allow the measurement of chemical changes in phases present in the tuff before reaction as well as the identification and chemical analysis of secondary phases resulting from hydrothermal reactions; and demonstrate the usefulness of geochemical modeling in a repository environment using the EQ3/6 thermodynamic/kinetic geochemical modeling code. Crushed tuff and polished wafers of tuff were reacted with a natural ground water in Dickson-type gold-cell rocking autoclaves which were periodically sampled under insitu conditions. Results were compared with predictions based on the EQ3/6 geochemical modeling code. Eight short-term experiments (2 to 3 months) at 150°C and 250°C have been completed using tuff from both drillcore and outcrop. Long-term experiments at 90°C and 150°C using drillcore polished wafers are in progress. This paper will focus on the results of the 150°C and 250°C experiments using drillcore polished wafers.

Geoengineering Characterization of Welded Tuffs from Laboratory and Field Investigations

AbstractWelded tuff beneath Yucca Mountain adjacent to the Nevada Test Site (NTS) is being considered for development as a high-level radioactive waste repository by the Nevada Nuclear Waste Storage Investigations (NNWSI) Project. Because access into Yucca Mountain has been limited to borehole explorations, early geoengineering materials characterizations have been derived From laboratory tests on cores from Yucca Mountain and from laboratory and field tests on welded tuffs located in G-Tunnel on the NTS. G-Tunnel contains welded tuffs that have similar properties and stress states to those at Yucca Mountain and has been the location for in situ rock mechanics testing. The purpose of this paper is to summarize the geoengineering material property data obtained to date and to compare appropriate laboratory and field data from G-Tunnel to findings from Yucca Mountain.Geomechanical and thermal data are provided and are augmented by limited geological and hydrological data. A comparison of results of laboratory measurements on tuffs from Yucca Mountain and G-Tunnel indicates good agreement between the bulk densities, saturations, moduli of elasticity, Poisson's ratios, and P-wave velocities. The G-Tunnel tuff has slightly lower thermal conductivity, tensile strength, compressive strength and slightly higher matrix permeability than does the welded tuff near the proposed repository horizon at Yucca Mountain. From a laboratory-to-field scaling perspective, the modulus of deformation shows the most sensitivity to field conditions because of the presence of joints found in the field.

Permeability and Pore-Fluid Chemistry of the Topopah Spring Member of the Paintbrush Tuff, Nevada Test Site, in a Temperature Gradient – Application to Nuclear Waste Storage

ABSTRACTThe Topopah Spring Member of the Paintbrush Tuff from the Nevada Test Site is being investigated by the Nevada Nuclear Waste Storage Investigations project (NNWSI) as a possible nuclear waste repository host rock. Changes with time of the permeability and fluid chemistry of the Topopah Spring Member have been measured in samples subjected to a temperature gradient. Maximum temperatures of the imposed gradients ranged from 90° to 250°C; minimum temperatures were 36° to 83°C. Confining and pore pressures simulated a depth of about 1.2 km, which is greater than the proposed repository depth, but chosen for comparison with previous studies at these pressures. Pore fluid used in the experiments was groundwater from the Nevada Test Site; the direction of pore-fluid flow was from the high- to the low-temperature side of the tuffs.Initial permeabilities of the tuff samples ranged from 3 to 65 μdarcys, the wide range in values resulting from differences in the void and fracture geometries of the samples. Heating the tuffs produced no change in permeability in tne lowest temperature experiment and only small changes at higher temperatures. The fluids discharged from the tuffs were dilute waters of nearneutral pH that differed only slightly from the original groundwater composition.Since proposed burial in the Topopah Spring Member would be in the unsaturated zone, the high initial permeabilities and the absence of permeability change with heating may be desirable, because downward-percolating waters would be able to drain into deeper formations and not collect at the repository level. in addition, any fluids that may come in contact with waste canisters wlll not have acquired any potentially corrosive characteristics through interaction with the tuff.

Post Emplacement Environment of Waste Packages

ABSTRACTExperiments have been conducted as part of the Nevada Nuclear Waste Storage Investigations Project to determine the changes in water chemistry due to reaction of the Topopah Spring tuff with natural groundwater at temperatures up to 150°C. The reaction extent has been investigated as a function of rock-to-water ratio, temperature, reaction time, physical state of the samples, and geographic location of the samples within the tuff unit. Results of these experiments will be used to provide information on the water chemistry to be expected if a high level waste repository were to be constructed in the Topopah Spring tuff.

NNWSI Performance Assessment Considerations

ABSTRACTThe Nevada Nuclear Waste Storage Investigations (NNWSI) project includes a Performance Assessment task to evaluate the containment and isolation potential for a nuclear waste repository at Yucca Mountain in southern Nevada. This task includes calculations of the rates and concentrations at which radionuclides might be released and transported from the repository and will predict their consequences if they enter the human environment. Among the major tasks required for these calculations will be the development of models for water flow and nuclide transport under unsaturated conditions and in fractured hard rock. The program must also quantify the uncertainties associated with the results of the calculations. The performance assessment will provide evaluations needed for making major decisions as the U. S. Department of Energy seeks a site for a repository. An evaluation will be part of the environmental assessments prepared to accompany the potential nomination of the site. If the Yucca mountain site is selected for characterization and development as a repository, the assessments will be required for an environmental impact statement, a safety analysis report, and other documents.This program has been divided into five tasks. Collectively they will provide the performance assessments needed for the NNWSI Project.

Selection of Barrier Metals for a Waste Package in Tuff

ABSTRACTThe Nevada Nuclear Waste Storage Investigations (NNWSI) project under the Civilian Radioactive Waste Management Program is planning a repository at Yucca Mountain at the Nevada Test Site for isolation of high-level nuclear waste. Lawrence Livermore National Laboratory is developing designs for an engineered barrier system containing several barriers such as the waste form, a canister and/or an overpack, packing, and near field host rock. In this paper we address the selection of metal containment barriers.