Phase stability of U5Si4, USi, and U2Si3 in the uranium-silicon system

JOURNAL OF NUCLEAR MATERIALS

卷:540

Article

Ulrich, Tashiema L.^1,2  Vogel, Sven C.²  Lopes, Denise A.^1,4  Kocevski, Vancho^1,2  White, Joshua T.²  Sooby, Elizabeth S.³  Besmann, Theodore M.¹ 

[1] Univ South Carolina, Mech Engn Dept, Nucl Engn Program, 541 Main ST, Columbia, SC 29201 USA

[2] Los Alamos Natl Lab, Mat Sci & Technol Div, MST 8,POB 1663, Los Alamos, NM 87544 USA

[3] Univ Texas San Antonio, Dept Phys & Astron, One UTSA Circle, San Antonio, TX 78249 USA

[4] Westinghouse Elect Sweden AB, Branslegatan 1, S-72136 Vasteras, Sweden

关键词: Uranium silicide;    Nuclear fuel;    Phase stability;    Crystal structure;   

DOI  :  10.1016/j.jnucmat.2020.152353

来源: Elsevier

【 摘 要 】

The intermetallic compound U3Si2 has received interest in recent years for use as accident tolerant fuels in light water reactors due to its combination of high thermal conductivity, reasonably high melting point, and high uranium density compared to UO2. Although U3Si2 is well characterized there are ucertainties about the remaining phases in the U-Si system which could be potential fission products of the silicide fuel. In an effort to better detail the U-Si binary phase diagram, the 44-60 at.% Si region of the U-Si phase diagram was investigated experimentally by analyzing samples with nominal compositions U/Si = 5/4, U/Si = 1/1 and U/Si = 2/3 using SEM-EDS, XRD, and high temperature time-of-flight neutron diffraction, supported by DFT calculations. Both the U/Si = 5/4 and the U/Si = 2/3 samples were composed of two phases, U3Si2 + USi and USi + U3Si5 for U/Si = 5/4 and U/Si = 2/3, respectively. Both U5Si4 and U2Si3 were found from DFT calculations to have imaginary phonon frequencies and an enthalpy of formation above the U-Si convex hull, and thus likely to be thermodynamically unstable compared to the other phases, consistent with the experimental results. In the literature there are three different structures that are proposed for the USi phase, and for the first time, high temperature neutron diffraction measurements were collected on the compound synthesized with the U/Si = 1/1 composition to verify the correct structure. The structure of the USi phase was confirmed to be tetragonal with the 14/mmm space group from room temperature to 1100 degrees C. The USin crystal structure has 6 U atom sites and 8 Si atoms sites of which two are partially occupied. Published by Elsevier B.V.

【 授权许可】

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