Scenario development for safety assessment in deep geologic disposal of high-level radioactive waste and spent nuclear fuel: A review.

Radiation and radioactive substances result in the production of radioactive wastes which require safe management and disposal to avoid risks to human health and the environment. To ensure permanent safe disposal, the performance of a deep geological repository for radioactive waste is assessed against internationally agreed risk-based standards. Assessing postclosure safety of the future system's evolution includes screening of features, events, and processes (FEPs) relevant to the situation, their subsequent development into scenarios, and finally the development and execution of safety assessment (SA) models. Global FEP catalogs describe important natural and man-made repository system features and identify events and processes that may affect these features into the future. By combining FEPs, many of which are uncertain, different possible future system evolution scenarios are derived. Repository licensing should consider both the reference or "base" evolution as well as alternative futures that may lead to radiation release, pollution, or exposures. Scenarios are used to derive and consider both base and alternative evolutions, often through production of scenario-specific SA models and the recombination of their results into an assessment of the risk of harm. While the FEP-based scenario development process outlined here has evolved somewhat since its development in the 1980s, the fundamental ideas remain unchanged. A spectrum of common approaches is given here (e.g., bottom-up vs. top-down scenario development, probabilistic vs. bounding handling of uncertainty), related to how individual numerical models for possible futures are converted into a determination as to whether the system is safe (i.e., how aleatoric uncertainty and scenarios are integrated through bounding or Monte Carlo approaches).

Temperature and Pressure Dependence of Salt-Brine Dihedral Angles in the Subsurface.

Elevated temperature and pressure in the earth's subsurface alters the permeability of salt formations, due to changing properties of the salt-brine interface. Molecular dynamics (MD) simulations are used to investigate the mechanisms of temperature and pressure dependence of liquid-solid interfacial tensions of NaCl, KCl, and NaCl-KCl brines in contact with (100) salt surfaces. Salt-brine dihedral angles vary between 55 and 76° across the temperature (300-450 K) and pressure range (0-150 MPa) evaluated. Temperature-dependent brine composition results in elevated dihedral angles of 65-80°, which falls above the reported salt percolation threshold of 60°. Mixed NaCl-KCl brine compositions increased this effect. Elevated temperatures excluded dissolved Na+ ions from the interface, causing the strong temperature dependence of the liquid-solid interfacial tension and the resulting dihedral angle. Therefore, at higher temperature, pressure, and brine concentrations Na-Cl systems may underpredict the dihedral angle. Higher dihedral angles in more realistic mixed brine systems maintain low permeability of salt formations due to changes in the structure and energetics of the salt-brine interface.

Surface Energies and Structure of Salt-Brine Interfaces.

Permeability of salt formations is controlled by the equilibrium between the salt-brine and salt-salt interfaces described by the dihedral angle, which can change with the composition of the intergranular brine. Here, classical molecular dynamics (MD) simulations were used to investigate the structure and properties of the salt-brine interface to provide insight into the stability of salt systems. Mixed NaCl-KCl brines were investigated to explore differences in ion size on the surface energy and interface structure. Nonlinearity was noted in the salt-brine surface energy with increasing KCl concentration, and the addition of 10% KCl increased surface energies by 2-3 times (5.0 M systems). Size differences in Na+ and K+ ions altered the packing of dissolved ions and water molecules at the interface, impacting the surface energy. Additionally, ions at the interface had lower numbers of coordinating water molecules than those in the bulk and increased hydration for ions in systems with 100% NaCl or 100% KCl brines. Ultimately, small changes in brine composition away from pure NaCl altered the structure of the salt-brine interface, impacting the dihedral angle and the predicted equilibrium permeability of salt formations.

Semi-Analytical Modeling of Transient Stream Drawdown and Depletion in Response to Aquifer Pumping.

Analytical and semi-analytical models for stream depletion with transient stream stage drawdown induced by groundwater pumping are developed to address a deficiency in existing models, namely, the use of a fixed stream stage condition at the stream-aquifer interface. Field data are presented to demonstrate that stream stage drawdown does indeed occur in response to groundwater pumping near aquifer-connected streams. A model that predicts stream depletion with transient stream drawdown is developed based on stream channel mass conservation and finite stream channel storage. The resulting models are shown to reduce to existing fixed-stage models in the limit as stream channel storage becomes infinitely large, and to the confined aquifer flow with a no-flow boundary at the streambed in the limit as stream storage becomes vanishingly small. The model is applied to field measurements of aquifer and stream drawdown, giving estimates of aquifer hydraulic parameters, streambed conductance, and a measure of stream channel storage. The results of the modeling and data analysis presented herein have implications for sustainable groundwater management.

Nonlinear dynamics and instability of aqueous dissolution of silicate glasses and minerals.

Aqueous dissolution of silicate glasses and minerals plays a critical role in global biogeochemical cycles and climate evolution. The reactivity of these materials is also important to numerous engineering applications including nuclear waste disposal. The dissolution process has long been considered to be controlled by a leached surface layer in which cations in the silicate framework are gradually leached out and replaced by protons from the solution. This view has recently been challenged by observations of extremely sharp corrosion fronts and oscillatory zonings in altered rims of the materials, suggesting that corrosion of these materials may proceed directly through congruent dissolution followed by secondary mineral precipitation. Here we show that complex silicate material dissolution behaviors can emerge from a simple positive feedback between dissolution-induced cation release and cation-enhanced dissolution kinetics. This self-accelerating mechanism enables a systematic prediction of the occurrence of sharp dissolution fronts (vs. leached surface layers), oscillatory dissolution behaviors and multiple stages of glass dissolution (in particular the alteration resumption at a late stage of a corrosion process). Our work provides a new perspective for predicting long-term silicate weathering rates in actual geochemical systems and developing durable silicate materials for various engineering applications.

Unsaturated hydraulic conductivity models based on truncated lognormal pore-size distributions.

We develop a closed-form three-parameter model for unsaturated hydraulic conductivity associated with the Kosugi three-parameter lognormal moisture retention model. The model derivation uses a slight modification to Mualem's theory, which is nearly exact for nonclay soils. Kosugi's three-parameter lognormal moisture retention model uses physically meaningful parameters, but a corresponding closed-form relative hydraulic conductivity model has never been developed. The model is further extended to a four-parameter model by truncating the underlying pore-size distribution at physically permissible minimum and maximum pore radii. The proposed closed-form models are fitted to well-known experimental data to illustrate their utility. They have the same physical basis as Kosugi's two-parameter model, but are more general.

Krypton-81 in groundwater of the Culebra Dolomite near the Waste Isolation Pilot Plant, New Mexico.

The Waste Isolation Pilot Plant (WIPP) in New Mexico is the first geologic repository for disposal of transuranic nuclear waste from defense-related programs of the US Department of Energy. It is constructed within halite beds of the Permian-age Salado Formation. The Culebra Dolomite, confined within Rustler Formation evaporites overlying the Salado Formation, is a potential pathway for radionuclide transport from the repository to the accessible environment in the human-disturbed repository scenario. Although extensive subsurface characterization and numerical flow modeling of groundwater has been done in the vicinity of the WIPP, few studies have used natural isotopic tracers to validate the flow models and to better understand solute transport at this site. The advent of Atom-Trap Trace Analysis (ATTA) has enabled routine measurement of cosmogenic (81)Kr (half-life 229,000 yr), a near-ideal tracer for long-term groundwater transport. We measured (81)Kr in saline groundwater sampled from two Culebra Dolomite monitoring wells near the WIPP site, and compared (81)Kr model ages with reverse particle-tracking results of well-calibrated flow models. The (81)Kr model ages are ~130,000 and ~330,000 yr for high-transmissivity and low-transmissivity portions of the formation, respectively. Compared with flow model results which indicate a relatively young mean hydraulic age (~32,000 yr), the (81)Kr model ages imply substantial physical attenuation of conservative solutes in the Culebra Dolomite and provide limits on the effective diffusivity of contaminants into the confining aquitards.

Influence of pressure change during hydraulic tests on fracture aperture.

In a series of field experiments, we evaluate the influence of a small water pressure change on fracture aperture during a hydraulic test. An experimental borehole is instrumented at the Korea Atomic Energy Research Institute (KAERI) Underground Research Tunnel (KURT). The target fracture for testing was found from the analyses of borehole logging and hydraulic tests. A double packer system was developed and installed in the test borehole to directly observe the aperture change due to water pressure change. Using this packer system, both aperture and flow rate are directly observed under various water pressures. Results indicate a slight change in fracture hydraulic head leads to an observable change in aperture. This suggests that aperture change should be considered when analyzing hydraulic test data from a sparsely fractured rock aquifer.

Basin-scale transmissivity and storativity estimation using hydraulic tomography.

While tomographic inversion has been successfully applied to laboratory- and field-scale tests, here we address the new issue of scale that arises when extending the method to a basin. Specifically, we apply the hydraulic tomography (HT) concept to jointly interpret four multiwell aquifer tests in a synthetic basin to illustrate the superiority of this approach to a more traditional Theis analysis of the same tests. Transmissivity and storativity are estimated for each element of a regional numerical model using the geostatistically based sequential successive linear estimator (SSLE) inverse solution method. We find that HT inversion is an effective strategy for incorporating data from potentially disparate aquifer tests into a basin-wide aquifer property estimate. The robustness of the SSLE algorithm is investigated by considering the effects of noisy observations, changing the variance of the true aquifer parameters, and supplying incorrect initial and boundary conditions to the inverse model. Ground water flow velocities and total confined storage are used as metrics to compare true and estimated parameter fields; they quantify the effectiveness of HT and SSLE compared to a Theis solution methodology. We discuss alternative software that can be used for implementing tomography inversion.