Nuclear Energy Advanced Modeling and Simulation

129 Pages·2011·1.22 MB·English

SANDIA REPORT
SAND2011-0845
Unlimited Release
February 2011

Nuclear Energy Advanced Modeling and
Simulation (NEAMS) Waste Integrated
Performance and Safety Codes (IPSC):
FY10 Development and Integration

Geoff Freeze, J. Guadalupe Argüello, Julie Bouchard, Louise Criscenti,
Thomas Dewers, H. Carter Edwards, David Sassani, Peter A. Schultz, and Yifeng Wang

Prepared by
Sandia National Laboratories
Albuquerque, New Mexico 87185 and Livermore, California 94550

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ii
SAND2011-0845
Unlimited Release
February 2011

Nuclear Energy Advanced Modeling and
Simulation (NEAMS) Waste Integrated
Performance and Safety Codes (IPSC):
FY10 Development and Integration

Geoff Freeze, J. Guadalupe Argüello, Julie Bouchard, Louise Criscenti,
Thomas Dewers, H. Carter Edwards, David Sassani, Peter A. Schultz, and Yifeng Wang

Sandia National Laboratories
P.O. Box 5800
Albuquerque, New Mexico 87185-MS1369

Abstract

This report describes the progress in fiscal year 2010 in developing the Waste Integrated
Performance and Safety Codes (IPSC) in support of the U.S. Department of Energy (DOE)
Office of Nuclear Energy Advanced Modeling and Simulation (NEAMS) Campaign. The goal
of the Waste IPSC is to develop an integrated suite of computational modeling and simulation
capabilities to quantitatively assess the long-term performance of waste forms in the engineered
and geologic environments of a radioactive waste storage or disposal system. The Waste IPSC
will provide this simulation capability (1) for a range of disposal concepts, waste form types,
engineered repository designs, and geologic settings, (2) for a range of time scales and distances,
(3) with appropriate consideration of the inherent uncertainties, and (4) in accordance with robust
verification, validation, and software quality requirements.

Waste IPSC activities in fiscal year 2010 focused on specifying a challenge problem to
demonstrate proof of concept, developing a verification and validation plan, and performing an
initial gap analyses to identify candidate codes and tools to support the development and
integration of the Waste IPSC. The current Waste IPSC strategy is to acquire and integrate the
necessary Waste IPSC capabilities wherever feasible, and develop only those capabilities that
cannot be acquired or suitably integrated, verified, or validated. This year-end progress report
documents the FY10 status of acquisition, development, and integration of thermal-hydrologic-
chemical-mechanical (THCM) code capabilities, frameworks, and enabling tools and
infrastructure.

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ACKNOWLEDGEMENTS

This work was supported by the U.S. Department of Energy, Office of Nuclear Energy, Fuel
Cycle Research and Development Program, Advanced Modeling and Simulation Campaign.

Charles Bryan supported the THCM code capability gap analysis by compiling the list of
potentially relevant codes in Appendix A. Helpful review comments were provided by Pat
Brady.

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CONTENTS

1. INTRODUCTION..................................................................................................................... 1 
1.1.  Waste IPSC Overview .................................................................................................... 1 
2. WASTE IPSC TECHNICAL SCOPE .................................................................................... 3 
3. CHARACTERIZATION OF SUB-CONTINUUM PROCESSES ....................................... 9 
3.1.  Overview of Glass Waste Form Dissolution ................................................................ 10 
3.1.1.  Repository Settings – Why and When Glass Waste Form Dissolution is
Important ...................................................................................................................... 10 
3.1.2.  Context of Glass Degradation ......................................................................... 11 
3.1.3.  Current Understanding and Gap Identification ............................................... 15 
3.2.  Continuum-Scale Rate Models for Glass Dissolution .................................................. 20 
3.2.1.  Overview of Kinetic Dissolution Rate Expressions ........................................ 20 
3.2.2.  Quantification of Rate Law Parameters .......................................................... 23 
3.3.  Molecular-Level Studies of Dissolution ....................................................................... 24 
3.3.1.  Determination of Reaction Mechanisms ......................................................... 24 
3.3.2.  Quantum Mechanics Cluster Calculations ...................................................... 25 
3.3.3.  Classical Molecular Dynamics (MD) Models ................................................ 31 
3.3.4.  Kinetic Monte Carlo (MC) Models for Dissolution ....................................... 33 
3.3.5.  Stochastic Monte Carlo (MC) Models for Dissolution ................................... 33 
3.3.6.  Modeling Mesoscale Effects on Glass ............................................................ 42 
3.3.7.  Experimental Validation of Molecular Models .............................................. 44 
3.3.8.  Summary of Gaps in Upscaling Dissolution Processes .................................. 46 
3.4.  Verification, Validation, and Uncertainty Quantification ............................................. 47 
3.4.1.  Practices for Sub-Continuum-Scale Modeling ............................................... 47 
3.4.2.  Upscaling with Propagating Uncertainties ...................................................... 48 
3.4.3.  Validation Issues ............................................................................................. 48 
3.4.4.  Evidence Management .................................................................................... 49 
3.5.  Summary of Glass Waste Form Dissolution Modeling ................................................ 49 
4. MODELING AND SIMULATION OF CONTINUUM PROCESSES ............................. 53 
4.1.  Thermal-Hydrologic-Chemical Processes and Code Capabilities ................................ 53 
4.1.1.  Thermal Modeling .......................................................................................... 53 
4.1.2.  Hydrologic Modeling ...................................................................................... 54 
4.1.3.  Multicomponent Multiphase Reactive-Transport Modeling .......................... 55 
4.2.  Mechanical Processes and Code Capabilities ............................................................... 65 
4.2.1.  Governing Mechanical Equations ................................................................... 65 
4.2.2.  Mechanical Modeling ..................................................................................... 67 
4.3.  Preliminary Gap Analysis of THCM Code Capabilities ............................................... 67 

v
CONTENTS (cont.)

5. FRAMEWORKS AND INFRASTRUCTURE..................................................................... 73 
5.1.  Enabling Infrastructure and Foundational Services ...................................................... 73 
5.1.1.  Configuration Management ............................................................................ 74 
5.1.2.  Requirements Management ............................................................................ 74 
5.1.3.  Project Management ....................................................................................... 75 
5.2.  Analysis Workflow Framework .................................................................................... 75 
5.2.1.  Plan for Gap Analysis, Acquisition, and Development .................................. 75 
5.2.2.  Potential Collaborators .................................................................................... 76 
5.2.3.  Framework Components Needs and Goals ..................................................... 77 
5.2.4.  Survey of Existing Solutions .......................................................................... 84 
6. SUMMARY ............................................................................................................................. 87 
7. REFERENCES ........................................................................................................................ 89 
APPENDIX A: REACTIVE TRANSPORT CODES ............................................................... 1 

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FIGURES

Figure 2-1. Components of a generic disposal system. ................................................................. 4 
Figure 3-1. Schematic of Initial Attack Stage. ............................................................................. 13 
Figure 3-2. Schematic of Evolution Stage. .................................................................................. 13 
Figure 3-3. Schematic of Maturation Stage. ................................................................................ 14 
Figure 3-4. Time dependent alteration rate and extent for glass degradation. ............................. 15 
Figure 3-5. Schematic showing the compositional profiles through the layers on the glass
surface. .......................................................................................................................................... 16 
Figure 3-6. Schematic diagram of the processes occurring within the passivating reactive
interphase (PRI). ........................................................................................................................... 17 
Figure 3-7. Time and length scales of geochemical modeling. ................................................... 20 
Figure 3-8. Energy profile (kJ/mol) of the Si-O-Si hydrolysis reaction along the reaction
coordinates for the protonated, neutral, and deprotonated species. .............................................. 28 
Figure 3-9. Schematic of the Al-O -Si surface site in (a) protonated, (b) neutral, and
br
(c) deprotonated states. ................................................................................................................. 29 
Figure 3-10. Flowchart for steps involved in the stepwise dissolution algorithm. ...................... 35 
Figure 3-11. Simplified model of a dissolving feldspar surface. ................................................. 39 
Figure 5-1. Flow of modeling and simulation capabilities from Development ........................... 73 

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TABLES

Table 2-1. Groupings of Potential Waste Form Types .................................................................. 3 
Table 2-2. Groupings of Potential Disposal Concepts and Geologic Settings .............................. 4 
Table 5-1. Enabling Infrastructure – Tool Identification and Gap Analysis ............................... 74 

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ACRONYMS

AFM atomic force microscopy
ASC Advanced Simulation and Computing
ASCEM Advanced Simulation Capability for Environmental Management
CP-MAS cross-polarization magic-angle spinning
CT Capability Transfer
DOE U.S. Department of Energy
EBS Engineered Barrier System
ECT Enabling Computational Technologies
FEP feature, event, and process
FY fiscal year
FMM Fundamental Methods and Models
GTCC greater than class C waste
HLW high-level waste
HPC high performance computing
HTGR high-temperature gas-cooled reactor
IPSC Integrated Safety and Performance Codes
LHS Latin hypercube sampling
LTHLW lower than high-level waste
MC Monte Carlo
MD molecular dynamics
MDCF multi-mechanism deformation coupled fracture
MO-TST molecular orbital-transition state theory
MPP massively parallel processing
NE Nuclear Energy
NEAMS Nuclear Energy Advanced Modeling and Simulation
NMR nuclear magnetic resonance
ODE ordinary differential equation
PA performance assessment
PDE partial differential equation
PRI passivating reactive interphase
RI reactive interface
SEM scanning electron microscopy
SIA Sequential iterative approach
SIMS secondary ion mass spectrometry
SNIA Sequential non-iterative approach
SNL Sandia National Laboratories
THC thermal-hydrologic-chemical
THCM thermal-hydrologic-chemical-mechanical
THCMBR thermal-hydrologic-chemical-mechanical-biological-radiological
TST transition state theory
UFD Used Fuel Disposition
UNF used nuclear fuel
UQ uncertainty quantification

ix
ACRONYMS (cont.)

V&V verification and validation
VSI vertical scanning interferometry
VU Verification and Validation and Uncertainty Quantification
WIPP Waste Isolation Pilot Plant
XPS X-ray photoelectron spectroscopy
YMP Yucca Mountain Project

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