First-principles study of inert gas incorporation and migration in zirconium nitride

Journal Article · Wed Jun 15 04:00:00 EDT 2016 · Transactions of the American Nuclear Society

OSTI ID:22992104

Mei, Zhi-Gang; Yacout, Abdellatif M.; Kim, Yeon Soo; Hofman, Gerard ^[1]

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1. Argonne National Laboratory, 9700 South Cass Avenue, Argonne, IL 60439 (United States)

Uranium-Molybdenum alloy based fuels are the most promising fuel for the future high performance research reactors using low enriched uranium (LEU). However, when used in dispersion with aluminum, significant amount of interaction products form at the interface between the UMo fuel particle and the surrounding Al during in-pile tests which leads to non-acceptable swelling. To reduce the swelling in U-Mo/Al dispersion fuel at high burnups, different diffusion barrier coatings, e.g., ZrN, were deposited on the U-Mo particles to avoid the interaction between fuel particles and the Al matrix. These diffusion barrier coatings are very effective in reducing the formation of interaction layer and therefore the fuel swelling. So far, ZrN is selected as the candidate coating material for the European Dispersion Fuel program due to the superior thermophysical properties of ZrN. The thermodynamic and kinetic stability of ZrN coating with respect to Al and U-Mo has been studied by the current authors using density functional theory calculations. So far there are very few studies of the diffusion behaviors of inert gases in ZrN. A recent publication on irradiated (Pu,Zr)N reveals that the majority of fission-induced Xe is retained in the material, while He is release to the fuel pin to a large extent. This raises the questions on the underlying differences of inert gas behavior in nitride fuel. Therefore, the purpose of this study is to understand the incorporation and migration behavior of inert gases He, Kr and Xe in ZrN using density functional theory (DFT) based first-principles calculations. Using density-functional theory calculations we provided a systematic study of the incorporation and migration of fission gases in ZrN. We investigated the formation energies of several defects (vacancies, interstitials, divacancies, Frenkel pairs, and Schottky defects) and the incorporation energies of inert gases in these defects. Results show that the formation energies of point defects are strongly affected by the chemical potentials of N and Zr species. The energetically most favorable incorporation site for fission gases is found to be the first nearest neighbor Schottky defect, in which the fission gas atom sits at somewhere between the Zr and N vacancies. The predicted solution energies of rare gases, i.e, He, Kr and Xe, in ZrN, is almost linearly dependent on the atom size of inert gases. We compared the solution energy Xe in ZrN with several other nuclear materials with the same B1 structure (MX), e.g., TiN, UN and UC. The solution energies of Xe in MX are closely related to the size of vacancy sites. The potential migration mechanisms of Xe in ZrN include interstitial and vacancy-assisted diffusion. The calculations show that vacancies essentially act as Xe trapping sites. The migration behavior of Xe in N and Zr divacancy and Schottky defects were compared with that through tetrahedral interstitials. It is found that the migration barrier is much lower with the interstitial mechanism than those with the vacancy mechanism. Therefore, at low temperatures Xe diffusion in ZrN is mostly through the interstitial mechanism or existing grain boundaries while at high temperature volume diffusion could be preferred, i.e., diffusion with Zr and N vacancies. (authors)

• OSTI ID: 22992104
• Journal Information: Transactions of the American Nuclear Society, Journal Name: Transactions of the American Nuclear Society Journal Issue: 1 Vol. 114; ISSN 0003-018X
• Country of Publication: United States
• Language: English

Related Subjects

36 MATERIALS SCIENCE
ALUMINIUM
BURNUP
COATINGS
DENSITY FUNCTIONAL METHOD
DIFFUSION BARRIERS
ENRICHED URANIUM
FISSION
FISSION PRODUCTS
FORMATION HEAT
FUEL PARTICLES
GRAIN BOUNDARIES
INTERFACES
INTERSTITIALS
IRRADIATION
LAYERS
MOLYBDENUM ALLOYS
RARE GASES
RESEARCH REACTORS
SCHOTTKY DEFECTS
SWELLING
ZIRCONIUM
ZIRCONIUM NITRIDES