Statistically averaged molecular dynamics simulations of hydrogen diffusion in magnesium and magnesium hydrides
Abstract
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.
- Authors:
-
[1]
- Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
- Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
- Publication Date:
- Research Org.:
- Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
- Sponsoring Org.:
- USDOE National Nuclear Security Administration (NNSA)
- OSTI Identifier:
- 1762850
- Report Number(s):
- LLNL-JRNL-810622
Journal ID: ISSN 2475-9953; 1016444; TRN: US2206062
- Grant/Contract Number:
- AC52-07NA27344; NA0003525
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Physical Review Materials
- Additional Journal Information:
- Journal Volume: 4; Journal Issue: 10; Journal ID: ISSN 2475-9953
- Publisher:
- American Physical Society (APS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; Diffusion; dynamical phase transitions
Citation Formats
Spataru, C. D., Heo, T. W., Wood, B. C., Stavila, V., Kang, S., Allendorf, M. D., and Zhou, X. W. Statistically averaged molecular dynamics simulations of hydrogen diffusion in magnesium and magnesium hydrides. United States: N. p., 2020.
Web. doi:10.1103/physrevmaterials.4.105401.
Spataru, C. D., Heo, T. W., Wood, B. C., Stavila, V., Kang, S., Allendorf, M. D., & Zhou, X. W. Statistically averaged molecular dynamics simulations of hydrogen diffusion in magnesium and magnesium hydrides. United States. https://doi.org/10.1103/physrevmaterials.4.105401
Spataru, C. D., Heo, T. W., Wood, B. C., Stavila, V., Kang, S., Allendorf, M. D., and Zhou, X. W. Mon .
"Statistically averaged molecular dynamics simulations of hydrogen diffusion in magnesium and magnesium hydrides". United States. https://doi.org/10.1103/physrevmaterials.4.105401. https://www.osti.gov/servlets/purl/1762850.
@article{osti_1762850,
title = {Statistically averaged molecular dynamics simulations of hydrogen diffusion in magnesium and magnesium hydrides},
author = {Spataru, C. D. and Heo, T. W. and Wood, B. C. and Stavila, V. and Kang, S. and Allendorf, M. D. and Zhou, X. W.},
abstractNote = {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.},
doi = {10.1103/physrevmaterials.4.105401},
journal = {Physical Review Materials},
number = 10,
volume = 4,
place = {United States},
year = {Mon Oct 05 00:00:00 EDT 2020},
month = {Mon Oct 05 00:00:00 EDT 2020}
}
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