A first-principles study of hydrogen surface coverage on δ-Pu (100), (111), and (110) surfaces

Mullen, Ryan Gotchy; Goldman, Nir

doi:10.1063/5.0064515

Title: A first-principles study of hydrogen surface coverage on δ-Pu (100), (111), and (110) surfaces

Journal Article · 20 December 2021 · Journal of Chemical Physics

DOI: https://doi.org/10.1063/5.0064515 · OSTI ID:1844089

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Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)

Hydriding corrosion of plutonium leads to surface cracking, pitting, and ultimately structural failure. Laboratory experiments demonstrate that hydriding begins on the surface or near the subsurface of plutonium. However, there has not yet been a systematic evaluation of hydrogen surface coverage on plutonium. In this work, we compute the surface energies of the low facet surfaces of face-centered cubic δ-Pu. The adsorption free energies of expected hydrogen structures at low and high coverage are presented along with the likely progression for filling sites as the H₂ partial pressure increases. Implications for near-equilibrium pressure hydride nucleation and non-equilibrium millibar pressure hydriding are discussed.

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Research Organization:: Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)

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

Grant/Contract Number:: AC52-07NA27344

OSTI ID:: 1844089

Report Number(s):: LLNL-JRNL-823460; 1034836

Journal Information:: Journal of Chemical Physics, Journal Name: Journal of Chemical Physics Journal Issue: 23 Vol. 155; ISSN 0021-9606

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

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Title: A first-principles study of hydrogen surface coverage on δ-Pu (100), (111), and (110) surfaces

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