Statistically averaged molecular dynamics simulations of hydrogen diffusion in magnesium and magnesium hydrides

Spataru, C. D.; Heo, T. W.; Wood, B. C.; Stavila, V.; Kang, S.; Allendorf, M. D.; Zhou, X. W.

doi:10.1103/physrevmaterials.4.105401

Statistically averaged molecular dynamics simulations of hydrogen diffusion in magnesium and magnesium hydrides

Journal Article · Mon Oct 05 00:00:00 EDT 2020 · Physical Review Materials

DOI:https://doi.org/10.1103/physrevmaterials.4.105401· OSTI ID:1762850

Spataru, C. D. ^[1]; Heo, T. W. ^[2]; Wood, B. C. ^[2]; Stavila, V. ^[1]; Kang, S. ^[2]; Allendorf, M. D. ^[1]; ^[1]

Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)

Magnesium has a different crystal structure from its dihydride with hydrogenation leading to a phase transition from the hexagonal closely packed Mg into a tetragonal α-MgH₂ rutile type structure. Such materials exhibit complex hydrogen uptake and release kinetics because hydrogen diffusivities significantly change when the crystal structure changes. To provide a foundational understanding of (de)hydrogenation kinetics that is applicable to all stages of the reaction, we performed statistically averaged molecular dynamics simulations to derive hydrogen diffusivities as a function of temperature and hydrogen content for both magnesium and magnesium hydride. Furthermore, our studies confirm that hydrogen diffusivities in magnesium hydride are much lower than in magnesium, in agreement with experimental data. Additionally, we observe that in either magnesium or magnesium hydride, higher hydrogen compositions result in reduced diffusivities. The latter was not revealed by prior experiments, which were conducted at fixed hydrogen composition. Finally, we discover a non-Arrhenius behavior in magnesium hydride. The physical origin of this behavior is also discussed.

View Accepted Manuscript (DOE)

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

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

Grant/Contract Number:: AC52-07NA27344; NA0003525

OSTI ID:: 1762850

Report Number(s):: LLNL-JRNL--810622; 1016444

Journal Information:: Physical Review Materials, Journal Name: Physical Review Materials Journal Issue: 10 Vol. 4; ISSN 2475-9953

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

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