The shock Hugoniot for full-density and porous CeO2 was investigated in the liquid regime using ab initio molecular dynamics (AIMD) simulations with Erpenbeck's approach based on the Rankine-Hugoniot jump conditions. The phase space was sampled by carrying out NVT simulations for isotherms between 6000 and 100 000 K and densities ranging from ρ=2.5 to 20g/cm3. The impact of on-site Coulomb interaction corrections +U on the equation of state (EOS) obtained from AIMD simulations was assessed by direct comparison with results from standard density functional theory simulations. Classical molecular dynamics (CMD) simulations were also performed to model atomic-scale shock compression of larger porous CeO2 models. Results from AIMD and CMD compression simulations compare favorably with Z-machine shock data to 525 GPa and gas-gun data to 109 GPa for porous CeO2 samples. Using results from AIMD simulations, an accurate liquid-regime Mie-Grüneisen EOS was built for CeO2. In addition, a revised multiphase SESAME-Type EOS was constrained using AIMD results and experimental data generated in this work. This study demonstrates the necessity of acquiring data in the porous regime to increase the reliability of existing analytical EOS models.
In this report, we present a thermodynamic-based model of hydride precipitation in Zr-based claddings. The model considers the state of the cladding immediately following drying, after removal from cooling-pools, and presents the evolution of precipitate formation upon cooling as follows: The pilgering process used to form Zr-based cladding imparts strong crystallographic and grain shape texture, with the basal plane of the hexagonal α-Zr grains being strongly aligned in the rolling-direction and the grains are elongated with grain size being approximately twice as long parallel to the rolling direction, which is also the long axis of the tubular cladding, as it is in the orthogonal directions.
The elastic properties and mechanical stability of zirconium alloys and zirconium hydrides have been investigated within the framework of density functional perturbation theory. Results show that the lowest-energy cubic Pn3m polymorph of δ-ZrH1.5 does not satisfy all the Born requirements for mechanical stability, unlike its nearly degenerate tetragonal P42/mcm polymorph. Elastic moduli predicted with the Voigt-Reuss-Hill approximations suggest that mechanical stability of α-Zr, Zr-alloy and Zr-hydride polycrystalline aggregates is limited by the shear modulus. According to both Pugh's and Poisson's ratios, α-Zr, Zr-alloy and Zr-hydride polycrystalline aggregates can be considered ductile. The Debye temperatures predicted for γ-ZrH, δ-ZrH1.5 and ε-ZrH2 are D = 299.7, 415.6 and 356.9 K, respectively, while D = 273.6, 284.2, 264.1 and 257.1 K for the α-Zr, Zry-4, ZIRLO and M5 matrices, i.e. suggesting that Zry-4 possesses the highest micro-hardness among Zr matrices.
This report documents the development, demonstration and validation of a mesoscale, microstructural evolution model for simulation of zirconium hydride {delta}-ZrH{sub 1.5} precipitation in the cladding of used nuclear fuels that may occur during long-term dry storage. While the Zr-based claddings are manufactured free of any hydrogen, they absorb hydrogen during service, in the reactor by a process commonly termed ‘hydrogen pick-up’. The precipitation and growth of zirconium hydrides during dry storage is one of the most likely fuel rod integrity failure mechanisms either by embrittlement or delayed hydride cracking of the cladding. While the phenomenon is well documented and identified as a potential key failure mechanism during long-term dry storage (NUREG/CR-7116), the ability to actually predict the formation of hydrides is poor. The model being documented in this work is a computational capability for the prediction of hydride formation in different claddings of used nuclear fuels. This work supports the Used Fuel Disposition Research and Development Campaign in assessing the structural engineering performance of the cladding during and after long-term dry storage. This document demonstrates a basic hydride precipitation model that is built on a recently developed hybrid Potts-phase field model that combines elements of Potts-Monte Carlo and the phase-field models. The model capabilities are demonstrated along with the incorporation of the starting microstructure, thermodynamics of the Zr-H system and the hydride formation mechanism.