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Experimental and computational assessment of U-Si-N ternary phases
KTH, School of Engineering Sciences (SCI), Physics, Nuclear Engineering.
Univ South Carolina, Columbia, SC 29208 USA..
Univ South Carolina, Columbia, SC 29208 USA..
Univ South Carolina, Columbia, SC 29208 USA..
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2019 (English)In: Journal of Nuclear Materials, ISSN 0022-3115, E-ISSN 1873-4820, Vol. 516, p. 194-201Article in journal (Refereed) Published
Abstract [en]

Uranium nitride-silicide composites are being considered as a high-density and high thermal conductivity fuel option for light water reactors. During development, chemical interactions were observed near the silicide melting point which resulted in formation of an unknown U-Si-N ternary phase. In the present work, U-Si-N composite samples were produced by arc-melting U3Si2 under an argon-nitrogen atmosphere to form the ternary phase. The resulting samples were characterized by SEM/EDS-EPMA and XRD, and demonstrated an equilibrium between U3Si2, UN, USi and a U-Si-N phase with a distinct crystallographic structure. Rietveld refinement of the ternary structure was performed, considering the ternary structures existent in the analogue U-Si-C system, and a good fit was obtained for the hexagonal U(20)Si(16)N(3 )phase. DFT + U calculations were performed in parallel to evaluate the thermodynamic and dynamic stability of the ternaries U20Si16N3 and U3Si2N2. The calculated enthalpy of formation and phonon dispersion support the existence of stable U20Si16N3 and U3Si2N2, although some soft modes in the U(20)Si(16)N(3)( )phase phonons are observed. The results presented here thus demonstrate the occurrence of at least one ternary phase in the U-Si-N system.

Place, publisher, year, edition, pages
Elsevier, 2019. Vol. 516, p. 194-201
National Category
Materials Chemistry
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URN: urn:nbn:se:kth:diva-245888DOI: 10.1016/j.jnucmat.2019.01.008ISI: 000458897100019Scopus ID: 2-s2.0-85060226032OAI: oai:DiVA.org:kth-245888DiVA, id: diva2:1295226
Note

QC 20190811

Available from: 2019-03-11 Created: 2019-03-11 Last updated: 2019-03-11Bibliographically approved

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