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Title: Molecular dynamics studies of fundamental bulk properties of palladium hydrides for hydrogen storage

Abstract

Solid-state hydrogen storage materials undergo complex phase transformations whose behavior are collectively determined by thermodynamic (e.g., Gibbs free energy), mechanical (e.g., lattice and elastic constants), and mass transport (e.g., diffusivity) properties. These properties depend on the reaction conditions and evolve continuously during (de)hydrogenation. Thus, they are difficult to measure in experiments. Because of this, past progress to improve solid-state hydrogen storage materials has been prolonged. Using PdH x as a representative example for interstitial metal hydride, we have recently applied molecular dynamics simulations to quantify hydrogen diffusion in the entire reaction space of temperature and composition. In this paper, we have further applied molecular dynamics simulations to obtain well-converged expressions for lattice constants, Gibbs free energies, and elastic constants of PdH x at various stages of the reaction. Finally, our studies confirm significant dependence of elastic constants on temperature and composition. Specifically, a new dynamic effect of hydrogen diffusion on elastic constants is discovered and discussed.

Authors:
ORCiD logo [1];  [2];  [2];  [1];  [2];  [1]
  1. Sandia National Lab. (SNL-CA), Livermore, CA (United States)
  2. Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
Publication Date:
Research Org.:
Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States); Sandia National Lab. (SNL-CA), Livermore, CA (United States)
Sponsoring Org.:
USDOE National Nuclear Security Administration (NNSA); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Fuel Cell Technologies Office (EE-3F)
OSTI Identifier:
1461752
Alternate Identifier(s):
OSTI ID: 1454296; OSTI ID: 1477976
Report Number(s):
LLNL-JRNL-705745; SAND-2016-11086J
Journal ID: ISSN 0021-8979; 840624; TRN: US1902036
Grant/Contract Number:  
AC52-07NA27344; NA0003525; AC04-94AL85000
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Applied Physics
Additional Journal Information:
Journal Volume: 123; Journal Issue: 22; Journal ID: ISSN 0021-8979
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
08 HYDROGEN; thermodynamic functions; phase transitions; transition metals; hydrogen storage; elastic moduli; molecular dynamics; mass diffusion; chemical compounds

Citation Formats

Zhou, X. W., Heo, T. W., Wood, B. C., Stavila, V., Kang, S., and Allendorf, M. D. Molecular dynamics studies of fundamental bulk properties of palladium hydrides for hydrogen storage. United States: N. p., 2018. Web. doi:10.1063/1.5022190.
Zhou, X. W., Heo, T. W., Wood, B. C., Stavila, V., Kang, S., & Allendorf, M. D. Molecular dynamics studies of fundamental bulk properties of palladium hydrides for hydrogen storage. United States. doi:10.1063/1.5022190.
Zhou, X. W., Heo, T. W., Wood, B. C., Stavila, V., Kang, S., and Allendorf, M. D. Thu . "Molecular dynamics studies of fundamental bulk properties of palladium hydrides for hydrogen storage". United States. doi:10.1063/1.5022190. https://www.osti.gov/servlets/purl/1461752.
@article{osti_1461752,
title = {Molecular dynamics studies of fundamental bulk properties of palladium hydrides for hydrogen storage},
author = {Zhou, X. W. and Heo, T. W. and Wood, B. C. and Stavila, V. and Kang, S. and Allendorf, M. D.},
abstractNote = {Solid-state hydrogen storage materials undergo complex phase transformations whose behavior are collectively determined by thermodynamic (e.g., Gibbs free energy), mechanical (e.g., lattice and elastic constants), and mass transport (e.g., diffusivity) properties. These properties depend on the reaction conditions and evolve continuously during (de)hydrogenation. Thus, they are difficult to measure in experiments. Because of this, past progress to improve solid-state hydrogen storage materials has been prolonged. Using PdHx as a representative example for interstitial metal hydride, we have recently applied molecular dynamics simulations to quantify hydrogen diffusion in the entire reaction space of temperature and composition. In this paper, we have further applied molecular dynamics simulations to obtain well-converged expressions for lattice constants, Gibbs free energies, and elastic constants of PdHx at various stages of the reaction. Finally, our studies confirm significant dependence of elastic constants on temperature and composition. Specifically, a new dynamic effect of hydrogen diffusion on elastic constants is discovered and discussed.},
doi = {10.1063/1.5022190},
journal = {Journal of Applied Physics},
number = 22,
volume = 123,
place = {United States},
year = {2018},
month = {6}
}

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