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Hydrogen-Enhanced Vacancy Diffusion in Metals.

Jun-Ping Du1,2, W T Geng2,3, Kazuto Arakawa4

  • 1Center for Elements Strategy Initiative for Structural Materials, Kyoto University, Kyoto 606-8501, Japan.

The Journal of Physical Chemistry Letters
|August 14, 2020
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Summary
This summary is machine-generated.

Hydrogen atoms unexpectedly enhance vacancy diffusion in metals like copper and palladium. This occurs because hydrogen is attracted to the transition state of vacancy migration, lowering the energy barrier for diffusion.

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Area of Science:

  • Materials Science
  • Physical Chemistry
  • Computational Materials Science

Background:

  • Vacancy diffusion is a critical process in materials science, influencing properties and performance.
  • Hydrogen atoms are known to interact strongly with vacancies, and are conventionally thought to impede their movement.

Purpose of the Study:

  • To investigate the effect of hydrogen on vacancy diffusion mechanisms in copper (Cu) and palladium (Pd).
  • To elucidate the underlying physical principles governing hydrogen-vacancy interactions during diffusion.

Main Methods:

  • Utilized the potential-of-mean-force (PMF) method to study vacancy diffusion.
  • Employed ab initio grand canonical Monte Carlo (GCMC) simulations.
  • Conducted direct molecular dynamics (MD) simulations for verification.

Main Results:

  • Contrary to expectations, hydrogen atoms were found to enhance vacancy diffusivity.
  • This enhancement is attributed to a positive hydrogen Gibbs excess at the migration saddle-point (activation excess ΓHm ≈ 1 H).
  • Positive migration activation volume (Ωm) and activation entropy (Sm) further support this finding.

Conclusions:

  • A higher chemical potential of hydrogen (μH) significantly reduces the migration free-energy barrier for vacancies.
  • The observed phenomenon is likely general for other migrating defects, including dislocations and grain boundaries, due to their positive activation volumes.
  • This study revises the understanding of hydrogen-vacancy interactions, highlighting a mechanism for enhanced diffusion.