Influence of Alloying Elements and Effect of Stress on Anisotropic Hydrogen Diffusion in Zr-Based Alloys Predicted by Accelerated Kinetic Monte Carlo Simulations

  • Jianguo YuEmail author
  • Chao Jiang
  • Yongfeng Zhang
Conference paper
Part of the The Minerals, Metals & Materials Series book series (MMMS)


The presence of hydrogen (H) can detrimentally affect the mechanical properties of many metals and alloys. To mitigate these detrimental effects requires fundamental understanding of the thermodynamics and kinetics governing H pickup and hydride formation. In this work, we focus on H diffusion in Zr-based alloys by studying the effects of alloying elements and stress, factors that have been shown to strongly affect H pickup and hydride formation in nuclear fuel claddings. A recently developed accelerated kinetic Monte Carlo method is used for the study. It is found that for the alloys considered here, H diffusivity depends weakly on composition, with negligible effect at high temperatures in the range of 600–1200 K. Therefore, the small variation in H diffusivity caused by variations in compositions of these alloys is likely not a major cause of the very different H pickup rates. In contrast, stress strongly affects H diffusivity. This effect needs to be considered for studying hydride formation and delayed hydride cracking.


Hydrogen diffusion Zirconium alloys Accelerated kinetic monte carlo 



We gratefully acknowledge the support of the Department of Energy (DOE) Nuclear Energy Advanced Modeling and Simulation (NEAMS) program. This manuscript has been authored by Battelle Energy Alliance, LLC under Contract No. DE-AC07-05ID14517 with the U.S. Department of Energy. The United States Government retains and the publisher, by accepting the article for publication, acknowledges that the United States Government retains a nonexclusive, paid-up, irrevocable, world-wide license to publish or reproduce the published form of this manuscript, or allow others to do so, for United States Government purposes.


  1. 1.
    A.T. Motta, A. Couet, R.J. Comstock, Corrosion of zirconium alloys used for nuclear fuel cladding. Annu. Rev. Mater. Res. 45, 311–343 (2015)CrossRefGoogle Scholar
  2. 2.
    S.J. Zinkle, K.A. Terrani, L.L. Snead, Motivation for utilizing new high-performance advanced materials in nuclear energy systems. Curr. Opin. Solid State Mater. Sci. 20, 401–410 (2016)CrossRefGoogle Scholar
  3. 3.
    T. Allen, R. Konings, A. Motta, Corrosion of zirconium alloys. Compreh. Nuclear Mater. 5, 49–68 (2012)CrossRefGoogle Scholar
  4. 4.
    K.S. Chan, An assessment of delayed hydride cracking in zirconium alloy cladding tubes under stress transients. Int. Mater. Rev. 58, 349–373 (2013)CrossRefGoogle Scholar
  5. 5.
    A. Sawatzky, The diffusion and solubility of hydrogen in the alpha-phase of zircaloy-2. J. Nucl. Mater. 2, 62–68 (1960)CrossRefGoogle Scholar
  6. 6.
    C.M. Schwartz, M.W. Mallett, Observations on the behavior of hydrogen in zirconium. Trans. Am. Soc. Metals 46, 640–654 (1954)Google Scholar
  7. 7.
    J.J. Kearns, Terminal solubility and partitioning of hydrogen in alpha phase of zirconium zircaloy-2 and zircaloy-4. J. Nucl. Mater. 22, 292–303 (1967)CrossRefGoogle Scholar
  8. 8.
    J.J. Kearns, Diffusion coefficient of hydrogen in α-Zr, Zircaloy2 and Zircaloy4. J. Nucl. Mater. 43, 330–338 (1972)CrossRefGoogle Scholar
  9. 9.
    C.S. Zhang, B. Li, P.R. Norton, The study of hydrogen segregation on Zr (0001) and Zr(10(1) over-bar0) surfaces by static secondary ion mass spectroscopy, work function, Auger electron spectroscopy and nuclear reaction analysis. J. Alloy. Compd. 231, 354–363 (1995)CrossRefGoogle Scholar
  10. 10.
    D.S. Sholl, Using density functional theory to study hydrogen diffusion in metals: a brief overview. J. Alloy. Compd. 446, 462–468 (2007)CrossRefGoogle Scholar
  11. 11.
    M. Christensen, W. Wolf, C. Freeman, E. Wimmer, R.B. Adamson, L. Hallstadius, P.E. Cantonwine, E.V. Mader, H in alpha-Zr and in zirconium hydrides: solubility, effect on dimensional changes, and the role of defects. J. Phys.-Conden. Matter 27, 025402 (2015)CrossRefGoogle Scholar
  12. 12.
    C. Domain, R. Besson, A. Legris, Atomic-scale Ab-initio study of the Zr-H system: i bulk properties. Acta. Materialia. 50, 3513–3526 (2002)CrossRefGoogle Scholar
  13. 13.
    B. Puchala, M.L. Falk, K. Garikipati, An energy basin finding algorithm for kinetic Monte Carlo acceleration. J. Chem. Phys. 132, 134104 (2010)CrossRefGoogle Scholar
  14. 14.
    Y.F. Zhang, C. Jiang, X.M. Bai, Anisotropic hydrogen diffusion in alpha-Zr and Zircaloy predicted by accelerated kinetic Monte Carlo simulations. Sci. Rep. 7, 41033 (2017)CrossRefGoogle Scholar
  15. 15.
    J.P. Perdew, K. Burke, M. Ernzerhof, Generalized gradient approximation made simple. Phys. Rev. Lett. 77, 3865–3868 (1996)CrossRefGoogle Scholar
  16. 16.
    G. Kresse, J. Furthmuller, Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set. Phys. Rev. B 54, 11169–11186 (1996)CrossRefGoogle Scholar
  17. 17.
    R. Agarwal, D.R. Trinkle, Light-element diffusion in Mg using first-principles calculations: Anisotropy and elastodiffusion. Phys. Rev. B 94, 054106 (2016)CrossRefGoogle Scholar

Copyright information

© The Minerals, Metals & Materials Society 2019

Authors and Affiliations

  1. 1.Fuels Modeling and SimulationIdaho National LaboratoryIdaho FallsUSA

Personalised recommendations