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Title: Temperature- and composition-dependent hydrogen diffusivity in palladium from statistically-averaged molecular dynamics

Abstract

Solid-state hydrogen storage materials undergo complex phase transformations whose kinetics is often limited by hydrogen diffusion. Among metal hydrides, palladium hydride undergoes a diffusional phase transformation upon hydrogen uptake, during which the hydrogen diffusivity varies with hydrogen composition and temperature. Here we perform robust statistically-averaged molecular dynamics simulations to obtain a well-converged analytical expression for hydrogen diffusivity in bulk palladium that is valid throughout all stages of the reaction. Our studies confirm significant dependence of the diffusivity on composition and temperature that elucidate key trends in the available experimental measurements. Whereas at low hydrogen compositions, a single process dominates, at high hydrogen compositions, diffusion is found to exhibit behavior consistent with multiple hopping barriers. Further analysis, supported by nudged elastic band computations, suggests that the multi-barrier diffusion can be interpreted as two distinct mechanisms corresponding to hydrogen-rich and hydrogen-poor local environments.

Authors:
 [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.:
Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
Sponsoring Org.:
USDOE National Nuclear Security Administration (NNSA)
OSTI Identifier:
1429694
Report Number(s):
SAND-2017-12692J
Journal ID: ISSN 1359-6462; 658955
Grant/Contract Number:  
AC04-94AL85000
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Scripta Materialia
Additional Journal Information:
Journal Volume: 149; Journal ID: ISSN 1359-6462
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Zhou, Xiaowang, Heo, Tae Wook, Wood, Brandon C., Stavila, Vitalie, Kang, Shinyoung, and Allendorf, Mark D. Temperature- and composition-dependent hydrogen diffusivity in palladium from statistically-averaged molecular dynamics. United States: N. p., 2018. Web. doi:10.1016/j.scriptamat.2018.02.010.
Zhou, Xiaowang, Heo, Tae Wook, Wood, Brandon C., Stavila, Vitalie, Kang, Shinyoung, & Allendorf, Mark D. Temperature- and composition-dependent hydrogen diffusivity in palladium from statistically-averaged molecular dynamics. United States. doi:10.1016/j.scriptamat.2018.02.010.
Zhou, Xiaowang, Heo, Tae Wook, Wood, Brandon C., Stavila, Vitalie, Kang, Shinyoung, and Allendorf, Mark D. Fri . "Temperature- and composition-dependent hydrogen diffusivity in palladium from statistically-averaged molecular dynamics". United States. doi:10.1016/j.scriptamat.2018.02.010.
@article{osti_1429694,
title = {Temperature- and composition-dependent hydrogen diffusivity in palladium from statistically-averaged molecular dynamics},
author = {Zhou, Xiaowang and Heo, Tae Wook and Wood, Brandon C. and Stavila, Vitalie and Kang, Shinyoung and Allendorf, Mark D.},
abstractNote = {Solid-state hydrogen storage materials undergo complex phase transformations whose kinetics is often limited by hydrogen diffusion. Among metal hydrides, palladium hydride undergoes a diffusional phase transformation upon hydrogen uptake, during which the hydrogen diffusivity varies with hydrogen composition and temperature. Here we perform robust statistically-averaged molecular dynamics simulations to obtain a well-converged analytical expression for hydrogen diffusivity in bulk palladium that is valid throughout all stages of the reaction. Our studies confirm significant dependence of the diffusivity on composition and temperature that elucidate key trends in the available experimental measurements. Whereas at low hydrogen compositions, a single process dominates, at high hydrogen compositions, diffusion is found to exhibit behavior consistent with multiple hopping barriers. Further analysis, supported by nudged elastic band computations, suggests that the multi-barrier diffusion can be interpreted as two distinct mechanisms corresponding to hydrogen-rich and hydrogen-poor local environments.},
doi = {10.1016/j.scriptamat.2018.02.010},
journal = {Scripta Materialia},
number = ,
volume = 149,
place = {United States},
year = {Fri Mar 09 00:00:00 EST 2018},
month = {Fri Mar 09 00:00:00 EST 2018}
}

Journal Article:
Free Publicly Available Full Text
This content will become publicly available on March 9, 2019
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Cited by: 1 work
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