Engineering topics

Wolery, Thomas J.

Publications and source records attributed to Wolery, Thomas J..

12 records

DOE OSTI2023

Evaluation of Nuclear Spent Fuel Disposal in Clay-Bearing Rock - Process Model Development and Experimental Studies

This report represents the milestone deliverable M2SF-23SN010301072 “Evaluation of Nuclear Spent Fuel Disposal in Clay-Bearing Rock - Process Model Development and Experimental Studies” The report provides a status update of FY23 activities for the work package Argillite Disposal work packages for the DOE-NE Spent Fuel Waste Form Science and Technology (SFWST) Program. Clay-rich geological media (often referred as shale or argillite) are among the most abundant type of sedimentary rock near the Earth’s surface. Argillaceous rock formations have the following advantageous attributes for deep geological nuclear waste disposal: widespread geologic occurrence, found in stable geologic settings, low permeability, self-sealing properties, low effective diffusion coefficient, high sorption capacity, and have the appropriate depth and thickness to host nuclear waste repository concepts. The DOE R&D program under the Spent Fuel Waste Science Technology (SFWST) campaign has made key progress (through experiment, modeling, and testing) in the study of chemical and physical phenomena that could impact the long-term safety assessment of heat-generating nuclear waste disposition in clay/shale/argillaceous rock. International collaboration activities comprising field-scale heater tests, field data monitoring, and laboratory-scale experiments provide key information on changes to the engineered barrier system (EBS) material exposed high thermal loads. Moreover, consideration of direct disposal of large capacity dual-purpose canisters (DPCs) as part of the back-end SNF waste disposition strategy has generated interest in improving our understanding of the effects of elevated temperatures on the engineered barrier system (EBS) design concepts. Chemical and structural analyses of sampled bentonite material from laboratory tests at elevated temperatures are key to the characterization of thermal effects affecting bentonite clay barrier performance. The knowledge provided by these experiments is crucial to constrain the extent of sacrificial zones in the EBS design during the thermal period. Thermal, hydrologic, mechanical, and chemical (THMC) data collected from heater tests and laboratory experiments have been used in the development, validation, and calibration of THMC simulators to model near-field coupled processes. This information leads to the development of simulation approaches to assess issues on coupled processes involving porous media flow, transport, geomechanical phenomena, chemical interactions with barrier/geologic materials, and the development of EBS concepts. These lines of knowledge are central to the design of deep geological backfilled repository concepts where temperature plays a key role in the EBS behavior, potential interactions with host rock, and long-term performance in the safety assessment.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2021

Evaluation of Nuclear Spent Fuel Disposal in Clay-Bearing Rock - Process Model Development and Experimental Studies (M2SF-21SN010301072)

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2020

Evaluation of Nuclear Spent Fuel Disposal in Clay-Bearing Rock - Process Model Development and Experimental Studies

The DOE R&D program under the Spent Fuel Waste Science Technology (SFWST) campaign has made key progress in modeling and experimental approaches towards the characterization of chemical and physical phenomena that could impact the long-term safety assessment of heat-generating nuclear waste disposition in deep clay/shale/argillaceous rock. International collaboration activities such as heater tests and postmortem analysis of samples recovered from these have elucidated key information regarding changes in the engineered barrier system (EBS) material exposed to years of thermal loads. Chemical and structural analyses of sampled bentonite material from such tests has as well as experiments conducted on these are key to the characterization of thermal effects affecting bentonite clay barrier performance and the extent of sacrificial zones in the EBS during the thermal period. Thermal, hydrologic, and chemical data collected from heater tests and laboratory experiments has been used in the development, validation, and calibration of THMC simulators to model near-field coupled processes. This information leads to the development of simulation approaches (e.g., continuum vs. discrete) to tackle issues related to flow and transport at various scales of the host-rock and EBS design concept. Consideration of direct disposal of large capacity dual-purpose canisters (DPCs) as part of the back-end SNF waste disposition strategy has generated interest in improving our understanding of the effects of elevated temperatures on the EBS design. This is particularly important for backfilled repository concepts where temperature plays a key role in the EBS behavior and long-term performance. This report describes multiple R&D efforts on disposal in argillaceous geologic media through development and application of coupled THMC process models, experimental studies on clay/metal/cement barrier and host-rock (argillite) material interactions, molecular dynamic (MD) simulations of water transport during (swelling) clay dehydration, first-principles studies of metaschoepite (UO 2 corrosion product) stability, and advances in thermodynamic plus surface complexation database development. Drift-scale URL experiments provides key data for testing hydrological-chemical (HC) model involving strong couplings of fluid mixing and barrier material chemical interactions. The THM modeling focuses on heater test experiments in argillite rock and gas migration in bentonite as part of international collaboration activities at underground research laboratories (URLs). In addition, field testing at an URL involves in situ analysis of fault slip behavior and fault permeability. Pore-scale modeling of gas bubble migration is also being investigated within the gas migration modeling effort. Interaction experiments on bentonite samples from heater test under ambient and elevated temperatures permit the evaluation of ion exchange, phase stability, and mineral transformation changes that could impact clay swelling. Advances in the development, testing, and implementation of a spent nuclear fuel (SNF) degradation model coupled with canister corrosion focus on the effects of hydrogen gas generation and its integration with Geologic Disposal Safety Assessment (GDSA). GDSA integration activities includes evaluation of groundwater chemistries in shale formations.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2020

H2OI95: A Stand-Alone Fortran Code for Evaluating the IAPWS-95 Equation-of-State Model for Water (Rev. 1)

H2OI95 is a stand-alone Fortran code for evaluating the IAPWS-95 equation-of-state model for the thermodynamic properties of water. It also evaluates the corresponding thermochemical properties of water consistent with the CODATA recommendations. The IAPWS-95 model is based on a model equation for the dimensionless Helmholtz energy for which the primary variables are the inverse reduced temperature (τ = T cr /T ) and reduced density (δ = ρ/ρ cr ). Here T is the absolute temperature (K), ρ is density (kg/m³), and the subscript “ cr ” refers to the critical point of water (647.096 K and 22.064 MPa pressure in this model, for which ρ cr is 322 kg/m³). The code solves four basic types of problems, distinguished by the specified inputs: 1. Temperature (K) and density (ρ kg/m³) or reduced density (δ) 2. Temperature (K) and pressure (MPa). 3. Temperature (K) on the saturation (liquid-vapor equilibrium) curve 4. Pressure (MPa) on the saturation curve. Each type of problem is run using a corresponding input (text) file. All but the first type of problem require iteration. For example, to solve for desired temperature and pressure, the reduced density must be adjusted to give the desired pressure. Iteration is accomplished using the Newton-Raphson method, though the secant method is also used in solving the fourth type of problem. For the last three types of problems, H2OI95 has been used to conduct numerical studies of convergence and the problem of multiple numerical solutions, some of which are not physically valid. Obtaining valid results depends mainly on appropriate choice of starting values for the density. The default values used in H2OI95 appear to consistently lead to generally desired results. With modification (not addressed here), H2OI95 can be used to support SUPCRT92 and similar codes that compute chemical thermodynamic properties of species and reactions over a wide range of temperature and pressure (273.16-1273K and 0-1000 MPa). Version 1.1 of this software calculates an extended set of water properties, including some derivable solely from IAPWS-95, such as the isobaric thermal expansivity and the isothermal compressibility, and still other properties based on supplementary models sanctioned by IAPWS, including the dynamic viscosity, thermal conductivity, surface tension, and static dielectric constant, and various other properties (notably Debye-Hückel parameters) derivable from the dielectric constant and its partial derivatives with respect to temperature and pressure. A coding error in Version 1.0 was identified while testing the implementation of the viscosity model. This error is described in Appendix C. It mainly affects calculation of “higher order” properties such as compressibility and heat capacity near the critical point.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2018

H2OI95: A Stand-Alone Fortran Code for Evaluating the IAPWS-95 Equation-of-State Model for Water

H2OI95 is a stand-alone Fortran code for evaluating the IAPWS-95 equation-of-state model (Wagner and Pruss, 2002) for the thermodynamic properties of water. It further evaluates the corresponding thermochemical properties of water consistent with the CODATA recommendations (Cox et al., 1989). The IAPWS-95 model is based on a model equation for the dimensionless Helmholtz energy for which the primary variables are the inverse reduced temperature (τ = T cr /T) and reduced density ( δ= ρ/ρ cr ). Here T is the absolute temperature (K), ρ is density (kg/m 3 ), and the subscript “cr” refers to the critical point of water (647.096 K and 22.064 MPa pressure in this model, for which ρ cr is 322 kg/m 3 ). The code solves four basic types of problems, distinguished by the specified inputs: 1, Temperature (K) and density (ρ kg/m 3 ) or reduced density (δ) 2. Temperature (K) and pressure (MPa). 3. Temperature (K) on the saturation (liquid-vapor equilibrium) curve 4. Pressure (MPa) on the saturation curve Each type of problem is run using a corresponding input (text) file. All but the first type of problem require iteration. For example, to solve for desired temperature and pressure, the reduced density must be adjusted to give the desired pressure. Iteration is accomplished using the Newton-Raphson method, though the secant method is also used in solving the fourth type of problem. H2OI95 has been used to conduct numerical studies of convergence and the problem of multiple numerical solutions, only some of which correspond to valid results. Obtaining valid results depends mainly on appropriate choice of starting values. The default values in H2OI95 appear to consistently lead to generally desired results. With modification (not addressed here), H2OI95 can be used to support SUPCRT92 (Johnson et al., 1992) and similar codes that compute chemical thermodynamic properties of species and reactions over a wide range of temperature and pressure (273.16-1273K and 0-1000 MPa).

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2017

Evaluation of Used Fuel Disposition in Clay-Bearing Rock

The DOE R&D program under the Spent Fuel Waste Science Technology (SFWST) campaign has made key advances in experimental and modeling aspects of chemical and physical phenomena towards the long-term safety assessment of nuclear waste disposition in deep clay/shale/argillaceous rock. Experimental activities on clay barrier interactions with fluids and radionuclides provide the much needed knowledge to evaluate engineered barrier system (EBS) performance. Thermal-Hydrological-Mechanical-Chemical (THMC) model development of clay provides a rigorous simulation platform to assess the complex dynamic behavior of engineered and natural barrier materials in response to coupled process phenomena induced by heat-generating nuclear waste. This report describes the ongoing disposal R&D efforts on the advancement and refinement of coupled THMC process models, hydrothermal experiments and geochemical modeling of on barrier material (clay/metal) interactions, spent fuel and canister material degradation, radiolytic phenomena and UO 2 degradation, and thermodynamic database development. These play an important role to the evaluation of sacrificial zones as part of the EBS exposure to thermally-driven chemical and transport processes. Clay-zeolite phase equilibria play a key role in the mineralogical transformations of clay barrier conducive to loss in swelling properties but also in controlling H 2 0 uptake/release through hydration/dehydration reactions. The result is volume changes can affect the interface / bulk phase porosities, transport, and the mechanical (stress) state of the bentonite barrier. Characterization studies on barrier samples (bentonite/cement) from controlled tests at underground research laboratories (URLs) provide key insights into barrier materials interactions at EBS interfaces. Spent fuel degradation modeling coupled with canister and cladding corrosion effects demonstrate the strong influence of H 2 generation on the source term.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2016

Chemical thermodynamic data. 1. The concept of links to the chemical elements and the historical development of key thermodynamic data [plus Supplementary Electronic Annex 2]

Chemical thermodynamic data remain a keystone for geochemical modeling and reactive transport simulation as applied to an increasing number of applications in the earth sciences, as well as applications in other areas including metallurgy, material science, and industrial process design. The last century has seen the development of a large body of thermodynamic data and a number of major compilations. The past several decades have seen the development of thermodynamic databases in digital form designed to support computer calculations. However, problems with thermodynamic data appear to be persistent. One problem pertains to the use of inconsistent primary key reference data. Such data pertain to elemental reference forms and key, stoichiometrically simple chemical species including metal oxides, CO 2 , water, and aqueous species such as Na + and Cl - . A consistent set of primary key data (standard Gibbs energies, standard enthalpies, and standard entropies for key chemical species) for 298.15K and 1 bar pressure is essential. Thermochemical convention is to define the standard Gibbs energy and the standard enthalpy of an individual chemical species in terms of formation from reference forms of the constituent chemical elements. We propose a formal concept of “links” to the elemental reference forms. This concept involves a documented understanding of all reactions and calculations leading to values for a formation property (standard Gibbs energy or enthalpy). A valid link consists of two parts: (a) the path of reactions and corrections and (b) the associated data, which are key data. Such a link differs from a bare “key” or “reference” datum in that it requires additional information. Some or all of its associated data may also be key data. In evaluating a reported thermodynamic datum, one should identify the links to the chemical elements, a process which can be time-consuming and which may lead to a dead end (an incomplete link). The use of two or more inconsistent links to the same elemental reference form in a thermodynamic database will result in an inconsistency in the database. Thus, in constructing a database, it is important to establish a set of reliable links (generally resulting in a set of primary reference data) and then correct all data adopted subsequently for consistency with that set. Recommended values of key data have not been constant through history. We review some of this history through the lens of major compilations and other influential reports, and note a number of problem areas. Finally, we illustrate the concepts developed in this paper by applying them to some key species of geochemical interest, including liquid water; quartz and aqueous silica; and gibbsite, corundum, and the aqueous aluminum ion.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2016

Evaluation of used fuel disposition in clay-bearing rock

The R&D program from the DOE Used Fuel Disposition Campaign (UFDC) has documented key advances in coupled Thermal-Hydrological-Mechanical-Chemical (THMC) modeling of clay to simulate its complex dynamic behavior in response to thermal and hydrochemical feedbacks. These efforts have been harnessed to assess the isolation performance of heat-generating nuclear waste in a deep geological repository in clay/shale/argillaceous rock formations. This report describes the ongoing disposal R&D efforts on the advancement and refinement of coupled THMC process models, hydrothermal experiments on barrier clay interactions, used fuel and canister material degradation, thermodynamic database development, and reactive transport modeling of the near-field under non-isothermal conditions. These play an important role to the evaluation of sacrificial zones as part of the EBS exposure to thermally-driven chemical and transport processes. Thermal inducement of chemical interactions at EBS domains enhances mineral dissolution/precipitation but also generates mineralogical changes that result in mineral H2O uptake/removal (hydration/dehydration reactions). These processes can result in volume changes that can affect the interface / bulk phase porosities and the mechanical (stress) state of the bentonite barrier. Characterization studies on bentonite barrier samples from the FEBEX-DP international activity have provided important insight on clay barrier microstructures (e.g., microcracks) and interactions at EBS interfaces. Enhancements to the used fuel degradation model outlines the need to include the effects of canister corrosion due the strong influence of H2 generation on the source term.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2016

Evaluation of used fuel disposition in clay-bearing rock.

The R&D program from the DOE Used Fuel Disposition Campaign (UFDC) has documented key advances in coupled Thermal-Hydrological-Mechanical-Chemical (THMC) modeling of clay to simulate its complex dynamic behavior in response to thermal and hydrochemical feedbacks. These efforts have been harnessed to assess the isolation performance of heatgenerating nuclear waste in a deep geological repository in clay/shale/argillaceous rock formations. This report describes the ongoing disposal R&D efforts on the advancement and refinement of coupled THMC process models, hydrothermal experiments on barrier clay interactions, used fuel and canister material degradation, thermodynamic database development, and reactive transport modeling of the near-field under non-isothermal conditions. These play an important role to the evaluation of sacrificial zones as part of the EBS exposure to thermallydriven chemical and transport processes. Thermal inducement of chemical interactions at EBS domains enhances mineral dissolution/precipitation but also generates mineralogical changes that result in mineral H2O uptake/removal (hydration/dehydration reactions). These processes can result in volume changes that can affect the interface / bulk phase porosities and the mechanical (stress) state of the bentonite barrier. Characterization studies on bentonite barrier samples from the FEBEX-DP international activity have provided important insight on clay barrier microstructures (e.g., microcracks) and interactions at EBS interfaces. Enhancements to the used fuel degradation model outlines the need to include the effects of canister corrosion due the strong influence of H 2 generation on the source term.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2015

Evaluation of Used Fuel Disposition in Clay-Bearing Rock

Deep geological disposal of nuclear waste in clay/shale/argillaceous rock formations has received much consideration given its desirable attributes such as isolation properties (low permeability), geochemically reduced conditions, slow diffusion, sorbtive mineralogy, and geologically widespread (Jové Colón et al., 2014). There is a wealth of gained scientific expertise on the behavior of clay/shale/ argillaceous rock given its focus in international nuclear waste repository programs that includes underground research laboratories (URLs) in Switzerland, France, Belgium, and Japan. Jové Colón et al. (2014) have described some of these investigative efforts in clay rock ranging from site characterization to research on the engineered barrier system (EBS). Evaluations of disposal options that include nuclear waste disposition in clay/shale/argillaceous rock have determined that this host media can accommodate a wide range of waste types. R&D work within the Used Fuel Disposition Campaign (UFDC) assessing thermal effects and fluid-mineral interactions for the disposition of heat-generating waste have so far demonstrated the feasibility for the EBS and clay host rock to withstand high thermal loads. This report represents the continuation of disposal R&D efforts on the advancement and refinement of coupled Thermal-Hydrological-Mechanical-Chemical (THMC), hydrothermal experiments on clay interactions, used fuel degradation (source term), and thermodynamic modeling and database development. The development and implementation of a clay/shale/argillite reference case described in Jové Colón et al. (2014) for FY15 will be documented in another report (Mariner et al. 2015) – only a brief description will be given here. This clay reference case implementation is the result of integration efforts between the GDSA PA and disposal in argillite work packages. The assessment of sacrificial zones in the EBS is being addressed through experimental work along with 1D reactive-transport and reaction path modeling. The focus of these investigations into the nature of sacrificial zones is to evaluate the chemical effects of heterogeneous chemical reactions at EBS interfaces. The difference in barrier material types and the extent of chemical reactions within these interfacial domains generates changes in mineral abundances. These mineralogical alterations also result in volume changes that, although small, could affect the interface bulk porosity. As in previous deliverables, this report is structured according to various national laboratory contributions describing R&D activities applicable to clay/shale/argillite media.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2011

FY11 Development of Fully Coupled Repository THCM Simulation Tools Report: Thermodynamic Database Development, with Emphasis on Complex Clay Minerals

Thermodynamic data are essential for understanding and evaluating geochemical processes, as by speciation-solubility calculations, reaction -path modeling, or reactive transport simulation. These data are required to evaluate both equilibrium states and the kinetic approach to such states (via the affinity term in rate laws). The development of thermodynamic databases for these purposes has a long history in geochemistry (e.g., Garrels and Christ, 1965; Helgeson et al., 1969; Helgeson et al., 1978, Johnson et al., 1992; Robie and Hemingway, 1995), paralleled by related and applicable work in the larger scientific community (e.g., Wagman et al., 1982, 1989; Cox et al., 1989; Barin and Platzki, 1995; Binneweis and Milke, 1999). The Yucca Mountain Project developed two qualified thermodynamic databases for to model geochemical processes, including ones involving repository components such as spent fuel. The first of the two (BSC, 2007a) was for systems containing dilute aqueous solutions only, the other (BSC, 2007b) for systems involving concentrated aqueous solutions and incorporating a model for such based on Pitzer’s (1991) equations . A 25°C-only database with similarities to the latter was also developed for WIPP (cf. Xiong, 2005). The YMP dilute systems database is widely used in the geochemistry community for a variety of applications involving rock/water interactions. The purpose of the present task is to improve these databases for work on the Used Fuel Disposition Project and maintain some semblance of order that will support qualification in support of the development of future underground high level nuclear waste disposal.

58 GEOSCIENCES↗

DOE OSTI2011

Disposal Systems Evaluation Framework (DSEF) Version 1.0 - Progress Report

The Disposal Systems Evaluation Framework (DSEF) is being developed at Lawrence Livermore National Laboratory to formalize the development and documentation of repository conceptual design options for each waste form and environment combination. This report summarizes current status and plans for the remainder of FY11 and for FY12. This progress report defines the architecture and interface parameters of the DSEF Excel workbook, which contains worksheets that link to each other to provide input and document output from external codes such that concise comparisons between fuel cycles, disposal environments, repository designs and engineered barrier system materials can be performed. Collaborations between other Used Fuel Disposition Campaign work packages and US Department of Energy / Nuclear Energy campaigns are clearly identified. File naming and configuration management is recommended to allow automated abstraction of data from multiple DSEF runs.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗