In situ High Temperature UO2 Grain Boundary and Bulk Mechanics under Irradiation

Principal Investigator
Name:
Shen Dillon
Email:
[email protected]
Phone:
(208) 526-6918
Team Members:
Name: Institution: Expertise: Status:
Brent Heuser University of Illinois at Urbana-Champaign Nuclear Materials Faculty
Andrew Nelson Oak Ridge National Laboratory Thermophysical Properties, Ceramics, ATF, Nuclear Fuel Other
Experiment Details:
Experiment Title:
In situ High Temperature UO2 Grain Boundary and Bulk Mechanics under Irradiation)
Hypothesis:
The grain boundary and lattice fracture toughness of undoped and doped UO2 are hypothesized to be affected by irradiation and gas implantation at temperatures relevant to fuel service. In the proposed work, the fracture toughness of these features are to be measured as a function of temperature and irradiation dose.
Work Description:
Bulk Cr2O3-doped and undoped UO2 samples have been provided by Oak Ridge National Laboratory. Microscale test specimen will be fabricated at the University of Illinois using Focused Ion Beam milling. Those samples will be mounted on appropriate Cu and Ti mounts, following procedures previously developed for high temperature testing of ZrO2 and UO2. These samples will be shipped to Sandia National Laboratories for testing. Mechanical tests will be performed using a Bruker Pi-95 nanomechanical tester. High temperatures will be achieved through laser heating with a 1 micron 20 W laser, which has been demonstrated in preliminary experiments to achieve the desired temperature range by ≈4 W focused on a 100-micron spot. Ion irradiations will be performed using MeV Cr ions irradiating samples <300-400 nm thick, which will enable most ions to penetrate the sample. Temperature will be calibrated through a combination of electron diffraction-based determination of thermal expansion and electrical resistance measurements. Notched cantilever fracture toughness measurements will be performed at ≈1000 oC, 1250 oC, and 1500 oC. Experiments will be performed as a function of dose at each temperature between 0 and 10 dpa using MeV Cr ion irradiation with and without ≈10 keV He implantation.
Project Summary
The overarching goal of the proposed work is to develop fundamental chemistry-structure-property relationships for UO2 grains and grain boundaries that serve as a basis for optimizing chemistry and engineering microstructure for damage tolerant fuels. Small scale testing will be employed in combination with in situ laser heating and ion irradiation with a goal of understanding and isolating the mechanical properties of individual microstructural features, e.g. the fracture toughness along specific crystallographic directions in the bulk and along grain boundaries, under conditions intended to model those experienced by fuels, T>1200 oC. The work builds on prior collaborations between the PI and Khalid Hattar’s group at Sandia National Laboratories where we have previously developed capabilities to perform in situ ion irradiation induced creep at high temperatures as well as in situ transmission electron microscopy based ultrahigh temperature, T>2000 oC, in situ mechanical testing. Experiments performed as a function of dopant chemistry, dose, and temperature will be used to develop fundamental structure-property relationships that will inform continuum scale mechanical models of fuels.
Relevance
Fabrication of samples used for this work is supported by the DOE-NE Advanced Fuels Campaign; within the goals of this broader effort our work is applying advanced characterization to improve the capability for development of science-based fuel development. Chemical additives (e.g. dopants) can be used to control the microstructure of UO2 fuels, which is an effective means to affect the distribution of fission gas product bubbles and related failures. Chemical additives in oxides may strongly influence mechanical properties and atomic diffusion at high temperatures. The effects of dopants on high temperature mechanical properties and high temperature properties under irradiation remain poorly defined. As a result, little data is available to inform or validate models necessary to predict damage evolution in doped fuels at high temperature under irradiation. This work will develop and demonstrate advanced characterization techniques that reasonably simulate fuel operating temperature, irradiation damage in terms of dpa and gas implantation, and irradiation flux. The effort will specifically focus on Cr2O3-doped UO2, which is a common additive in commercial fuels. The work scope addresses validation needs related to meso-scale microstructure evolution of UO2 in separate effects experimentation and is therefore coupled to Appendix D. It is envisioned that the single grain boundary and microstructural fracture toughness UO2 grain boundaries can provide validation for calculated data in BISON.
Book / Journal Publications

"Using in situ UO2 bicrystal sintering to understand grain boundary dislocation nucleation kinetics and creep" Shen Dillon, Journal of the American Ceramic Society 2024 Link