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Grain growth and pore coarsening in dense nano-crystalline UO2+x fuel pellets

Journal Article · · Journal of the American Ceramic Society
DOI:https://doi.org/10.1111/jace.14780· OSTI ID:1373755
 [1];  [2];  [3];  [1];  [2];  [1]
  1. Rensselaer Polytechnic Institute, Troy, NY (United States)
  2. Argonne National Lab. (ANL), Lemont, IL (United States)
  3. Argonne National Lab. (ANL), Lemont, IL (United States); Xi'an Jiaotong Univ., Shaanxi (China)

Dense nano-sized UO2+x pellets are synthesized by spark plasma sintering with controlled stoichiometries (UO2.03 and UO2.11) and grain sizes (~100 nm), and subsequently isothermally annealed to study their effects on grain growth kinetics and microstructure stability. The grain growth kinetics is determined and analyzed focusing on the interaction between grain boundary migration, pore growth and coalescence. Grains grow much bigger in nano-sized UO2.11 than UO2.03 upon thermal annealing, consistent with the fact that hyper-stoichiometric UO2+x is beneficial for sintering due to enhanced U ion diffusion from excessive O ion interstitials. The activation energies of the grain growth for UO2.03 and UO2.11 are determined as ~1.0 and 1.3~2.0 eV, respectively. As compared with the micron-sized UO2 in which volumetric diffusion dominates the grain coarsening with an activation energy of ~3.0 eV, the enhanced grain growth kinetics in nano-sized UO2+x suggests that grain boundary diffusion controls grain growth. Lastly, the higher activation energy of more hyper-stoichiometric nano-sized UO2.11 may be attributed to the excessive O interstitials pinning grain boundary migration.

Research Organization:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Organization:
USDOE Office of Nuclear Energy (NE), Nuclear Energy Advanced Modeling and Simulation (NEAMS); USDOE Office of Nuclear Energy (NE), Nuclear Energy University Programs (NEUP); National Science Foundation (NSF)
Grant/Contract Number:
AC02-06CH11357
OSTI ID:
1373755
Alternate ID(s):
OSTI ID: 1401771
Journal Information:
Journal of the American Ceramic Society, Journal Name: Journal of the American Ceramic Society Journal Issue: 6 Vol. 100; ISSN 0002-7820
Publisher:
American Ceramic SocietyCopyright Statement
Country of Publication:
United States
Language:
English

References (29)

Defect Structure and the Related Properties of UO2 and Doped UO2 book January 1989
Oxygen ion self-diffusion in uranium dioxide journal March 1961
Lattice and grain-boundary diffusion of uranium in UO2 journal August 1966
Grain growth in pure and titania-doped uranium dioxide journal March 1966
A study of cation diffusion in UO2 + x and ThO2 using α-ray spectrometry journal April 1968
Uranium and oxygen self-diffusion in UO2 journal April 1969
On uranium self-diffusion in UO2 and UO2+ journal April 1969
Isothermal grain growth kinetics in sintered UO2 pellets journal December 1973
Grain growth in UO2: in-reactor and laboratory testing journal July 1979
Investigation of the oxygen activity of oxide fuels and fuel-fission product systems by solid electrolyte techniques. Part I: Qualification and limitations of the method journal June 1983
Grain growth kinetics in uranium-plutonium mixed oxides journal January 1986
Activation energy of UO2 and UO2+x sintering journal December 2001
Effect of grain-boundaries on uranium and oxygen diffusion in polycrystalline UO2 journal April 2000
The high burn-up structure in nuclear fuel journal December 2010
An object-oriented finite element framework for multiphysics phase field simulations journal January 2012
High-pressure spark plasma sintering (SPS) of transparent polycrystalline magnesium aluminate spinel (PMAS) journal December 2014
Self-diffusion near symmetrical tilt grain boundaries in UO2 matrix: A molecular dynamics simulation study journal July 2009
Bulk-nanocrystalline oxide nuclear fuels – An innovative material option for increasing fission gas retention, plasticity and radiation-tolerance journal March 2012
An experimental study of grain growth in mixed oxide samples with various microstructures and plutonium concentrations journal March 2013
Phase field simulation of grain growth in porous uranium dioxide journal March 2014
Neutron Diffraction Study of the in Situ Oxidation of UO 2 journal August 2009
NIH Image to ImageJ: 25 years of image analysis journal June 2012
Average structure and local configuration of excess oxygen in UO2+x journal March 2014
Raman spectroscopic studies of defect structures and phase transition in hyper-stoichiometric UO2+x journal January 2010
Nuclear fuel in generation II and III reactors: research issues related to high burn-up journal January 2011
Influence of Stoichiometry on the Rate of Grain Growth of UO2 journal August 1963
Grain Growth in CeO2: Dopant Effects, Defect Mechanism, and Solute Drag journal July 1996
Grain Boundary Mobility in Y2O3: Defect Mechanism and Dopant Effects journal July 1996
NEAMS FPL M2 Milestone Report: Development of a UO₂ Grain Size Model using Multicale Modeling and Simulation report June 2014

Cited By (3)

Kinetic study on the grain growth of PuO 2 nanocrystals journal January 2019
Structural properties of ultra-small thorium and uranium dioxide nanoparticles embedded in a covalent organic framework journal January 2020
Consolidation of commercial-size UO2 fuel pellets using spark plasma sintering and microstructure/microchemical analysis journal July 2018

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