journal article·2022-08Open access

Structural and phase evolution in U3Si2 during steam corrosion

Jiatu Liu, Patrick A. Burr, Joshua T. White, Vanessa K. Peterson, Pranesh Dayal, Christopher Baldwin, Deborah Wakeham, Daniel J. Gregg, Elizabeth S. Sooby, Edward G. Obbard

Corrosion Science· Volume 204

Abstract

U$_3$Si$_2$ nuclear fuel is corroded in deuterated steam with in situ neutron diffraction. Density functional theory is coupled with rigorous thermodynamic description of the hydride including gas/solid entropy contributions. H absorbs in the 2$b$ interstitial site of U$_3$Si$_2$H$_x$ and moves to 8$j$ for $x\ge 0.5$. Hydriding forces lattice expansion and change in $a/c$ ratio linked to site preference. Rietveld refinement tracks the corrosion reactions at 350-500 °C and preference for the 8j site. Above 375 °C, formation of UO$_2$, U$_3$Si$_5$ and USi$_3$ take place in the grain boundaries and bulk. Hydriding occurs in bulk and precedes other reactions.
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Research context

OpenAlex topics: Nuclear Materials and Properties · Radioactive element chemistry and processing · Fusion materials and technologies

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References (37)

Show source-provided references
1. J.T. White, A.T. Nelson, J.T. Dunwoody, D.J. Safarik, K.J. McClellan, Corrigendum to “Thermophysical properties of U3Si2 to 1773 K” [J. Nucl. Mater. (2015) 464 (275–280)] (S002231151500241X)(10.1016/j.jnucmat.2015.04.031), Journal of Nuclear Materials. 484 (2017) 386–387. https://doi.org/10.1016/j.jnucmat.2016.11.015.10.1016/j.jnucmat.2016.11.015 ↗
2. Irradiation behaviour of uranium silicide compounds10.1016/j.jnucmat.2003.11.009 ↗
3. The Opal (Open Pool Australian Light-Water) Reactor in Australia
4. Challenges and opportunities to alloyed and composite fuel architectures to mitigate high uranium density fuel oxidation: uranium silicide10.1016/j.jnucmat.2021.153026 ↗
5. Thermal and mechanical properties of polycrystalline U3Si2 synthesized by spark plasma sintering10.1080/00223131.2018.1480431 ↗
6. Anisotropy in the thermal expansion of uranium silicide measured by neutron diffraction10.1016/j.jnucmat.2018.04.049 ↗
7. High temperature neutron diffraction investigation of U3Si210.1016/j.mtla.2019.100580 ↗
8. Gaseous swelling of U3Si2 during steady-state LWR operation: A rate theory investigation10.1016/j.nucengdes.2017.07.008 ↗
9. Non-stoichiometry in U3Si210.1016/j.jnucmat.2016.10.016 ↗
10. U3Si2 behavior in H2O: Part I, flowing steam and the effect of hydrogen10.1016/j.jnucmat.2018.01.002 ↗
11. Solution of hydrogen in accident tolerant fuel candidate material: U3Si210.1016/j.jnucmat.2018.01.018 ↗
12. The U3Si2 - H system10.1016/j.jnucmat.2021.153278 ↗
13. Wombat: The high-intensity powder diffractometer at the OPAL reactor10.1016/j.physb.2006.05.323 ↗
14. Certification of standard reference material 660B10.1154/1.3591064 ↗
15. A profile refinement method for nuclear and magnetic structures10.1107/S0021889869006558 ↗
16. General structure analysis system (GSAS)
17. Gsaslanguage: A GSAS script language for automated Rietveld refinements of diffraction data10.1107/S0021889811023181 ↗
18. Atomic radii in crystals10.1063/1.1725697 ↗
19. A new form of uranium hydride10.1021/ja01630a094 ↗
20. The hydrogen positions in uranium hydride by neutron diffraction10.1021/ja01153a035 ↗
21. Infrared spectrum of trideuterosilane and the structure of the silane molecule10.1063/1.1742148 ↗
22. Magnetic and electrical properties of the U-Si system (part II)10.1016/0304-8853(92)90697-M ↗
23. The oxidation of NiAl: what can we learn from ab initio calculations?10.1146/annurev.matsci.35.101503.091652 ↗
24. Haynes · 2016
25. Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set10.1103/PhysRevB.54.11169 ↗
26. From ultrasoft pseudopotentials to the projector augmented-wave method10.1103/PhysRevB.59.1758 ↗
27. Generalized gradient approximation made simple10.1103/PhysRevLett.77.3865 ↗
28. Electron-energy-loss spectra and the structural stability of nickel oxide: An LSDA+U study10.1103/PhysRevB.57.1505 ↗
29. Phase equilibria in the U-Si system from first-principles calculations10.1016/j.jnucmat.2016.07.006 ↗
30. Importance of elastic finite-size effects: Neutral defects in ionic compounds10.1103/PhysRevB.96.094107 ↗
31. Symmetry-adapted configurational modelling of fractional site occupancy in solids10.1088/0953-8984/19/25/256201 ↗
32. Modeling brittle fracture due to anisotropic thermal expansion in polycrystalline materials10.1016/j.commatsci.2021.110407 ↗
33. Oxidation and phase separation of U3Si2 nuclear fuel in high-temperature steam environments10.1016/j.jnucmat.2020.152517 ↗
34. Wyckoff · 1963
35. On the oxidation mechanism of U3Si2 accident tolerant nuclear fuel
36. High temperature steam oxidation dynamics of U3Si2 with alloying additions: Al, Cr, and Y
37. DFT + U Study of the adsorption and dissociation of water on clean, defective, and oxygen-Covered U3Si2{001}, {110}, and {111} Surfaces10.1021/acs.jpcc.9b03076 ↗