Ab Initio Simulations of Tritium Diffusion in Al-Rich Iron Aluminide Coating Phases

Sassi, Michel; Senor, David J.; Casella, Andrew M.

doi:10.1021/acs.jpcc.3c01028

Ab Initio Simulations of Tritium Diffusion in Al-Rich Iron Aluminide Coating Phases

Journal Article · Mon May 22 00:00:00 EDT 2023 · Journal of Physical Chemistry. C

DOI:https://doi.org/10.1021/acs.jpcc.3c01028· OSTI ID:1987498

^[1]; Senor, David J. ^[1]; ^[1]

Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Surface coatings of steels used in extreme conditions and corrosive environments generally aim to provide protection and increased durability. In the case of tritium-producing burnable absorber rods (TPBARs) used in nuclear reactors, a 316 stainless steel has been coated with Al. Scanning transmission electron microscopy (STEM) characterization of the coating found three Al-rich (>60 atom % Al) iron aluminide alloys identified as hexagonal FeNiAl₅, monoclinic Fe₄Al₁₃, and orthorhombic Fe₂Al₅. Density functional theory simulations using nudged elastic band have been performed to investigate the diffusion of interstitial tritium in each Al-rich iron aluminide phase. While FeNiAl₅ and Fe₄Al₁₃ can be viewed as the stacking of two layers, the structural peculiarity of Fe₂Al₅ is that channels of variable Al vacancy content are present along the c-axis. Therefore, three stoichiometries for Fe₂Al_x phase, namely, Fe₂Al₄, Fe₂Al₅, and Fe₂Al₆, have been considered to evaluate the impact of Al vacancy concentration on tritium diffusion behavior. Altogether, we found that at 600 K, tritium diffusion decreases from a faster rate in the channels of Fe₂Al_x phases (D_T ≤ 10^–11 m²·s^–1) to Fe₄Al₁₃ (D_T ≈ 10–12 m2·s–1), and finally in FeNiAl5 (D_T ≈ 10^–13 m²·s^–1). Here, we also find that interstitial tritium generally diffuses faster in Fe–Al coating phases than in the tritium breeding material γ-LiAlO₂ (D_T ≈ 10^–14 m²·s^–1) but slightly slower than in 316 stainless steel (D_T ≈ 10^–10 m²·s^–1).

View Accepted Manuscript (DOE)

Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: AC05-76RL01830

OSTI ID:: 1987498

Report Number(s):: PNNL-SA-181376

Journal Information:: Journal of Physical Chemistry. C, Journal Name: Journal of Physical Chemistry. C Journal Issue: 21 Vol. 127; ISSN 1932-7447

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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