Hexagonal close-packed high-entropy alloy formation under extreme processing conditions

We assess the validity of criteria based on size mismatch and thermodynamics in predicting the stability of the rare class of high-entropy alloys (HEAs) that form in the hexagonal close-packed crystal structure. We focus on nanocrystalline HEA particles composed predominantly of Mo, Tc, Ru, Rh, and Pd along with Ag, Cd, and Te, which are produced in uranium dioxide fuel under the extreme conditions of nuclear reactor operation. The constituent elements are fission products that aggregate under the combined effects of irradiation and elevated temperature as high as 1200 °C. We present the recent results on alloy nanoparticle formation in irradiated ceria, which was selected as a surrogate for uranium dioxide, to show that radiation-enhanced diffusion plays an important role in the process. This work sheds light on the initial stages of alloy nanoparticle formation from a uniform dispersion of individual metals. The remarkable chemical durability of such multiple principal element alloys presents a solution, namely, an alloy waste form, to the challenge of immobilizing Tc.

[1]  S. Zinkle,et al.  Irradiation responses and defect behavior of single-phase concentrated solid solution alloys , 2018, Journal of Materials Research.

[2]  M. Widom Modeling the structure and thermodynamics of high-entropy alloys , 2018, Journal of Materials Research.

[3]  Y. Estrin,et al.  Microstructure and Mechanical Properties of High-Entropy Alloy Co20Cr26Fe20Mn20Ni14 Processed by High-Pressure Torsion at 77 K and 300 K , 2018, Scientific Reports.

[4]  R. Arróyave,et al.  Probing the entropy hypothesis in highly concentrated alloys , 2018 .

[5]  M. Widom,et al.  Thermodynamics of concentrated solid solution alloys , 2017 .

[6]  M. Widom,et al.  Computational modeling of high-entropy alloys: Structures, thermodynamics and elasticity , 2017 .

[7]  L. Shao,et al.  Nanoparticle Precipitation in Irradiated and Annealed Ceria Doped with Metals for Emulation of Spent Fuels , 2017 .

[8]  M. Hanfland,et al.  First hexagonal close packed high-entropy alloy with outstanding stability under extreme conditions and electrocatalytic activity for methanol oxidation , 2017 .

[9]  S. Gorsse,et al.  Mapping the world of complex concentrated alloys , 2017 .

[10]  Jinyuan Yan,et al.  Polymorphism in a high-entropy alloy , 2017, Nature Communications.

[11]  P. Burr,et al.  DFT study of the hexagonal high-entropy alloy fission product system , 2017 .

[12]  R. Devanathan Molecular Dynamics Simulation of Fission Fragment Damage in Nuclear Fuel and Surrogate Material , 2017 .

[13]  A. Melnick,et al.  Thermodynamic design of high-entropy refractory alloys , 2017 .

[14]  Jing Zhu,et al.  Formation of Hexagonal-Close Packed (HCP) Rhodium as a Size Effect. , 2017, Journal of the American Chemical Society.

[15]  Hongbin Bei,et al.  High pressure synthesis of a hexagonal close-packed phase of the high-entropy alloy CrMnFeCoNi , 2016, Nature Communications.

[16]  D. Miracle,et al.  A critical review of high entropy alloys and related concepts , 2016 .

[17]  J. Crum,et al.  Options for the Separation and Immobilization of Technetium , 2016 .

[18]  Boliang Zhang,et al.  High-Entropy Alloys in Hexagonal Close-Packed Structure , 2016, Metallurgical and Materials Transactions A.

[19]  Yong Zhang,et al.  A hexagonal close-packed high-entropy alloy: The effect of entropy , 2016 .

[20]  N. Jones,et al.  High-entropy alloys: a critical assessment of their founding principles and future prospects , 2016 .

[21]  Daniel B. Miracle,et al.  A New Thermodynamic Parameter to Predict Formation of Solid Solution or Intermetallic Phases in High Entropy Alloys (Postprint) , 2016 .

[22]  A. G. McGregor,et al.  Predicting the formation and stability of single phase high-entropy alloys , 2016 .

[23]  D. Raabe,et al.  Ab initio thermodynamics of the CoCrFeMnNi high entropy alloy: Importance of entropy contributions beyond the configurational one , 2015 .

[24]  Edward J. Mausolf,et al.  Nanostructure of metallic particles in light water reactor used nuclear fuel , 2015 .

[25]  C. Trautmann,et al.  Characterization of swift heavy ion irradiation damage in ceria , 2015 .

[26]  Douglas L. Irving,et al.  A Novel Low-Density, High-Hardness, High-entropy Alloy with Close-packed Single-phase Nanocrystalline Structures , 2015 .

[27]  D. King,et al.  Atomic scale modelling of hexagonal structured metallic fission product alloys , 2015, Royal Society Open Science.

[28]  Paul R. C. Kent,et al.  Criteria for Predicting the Formation of Single-Phase High-Entropy Alloys , 2015 .

[29]  C. Woodward,et al.  Accelerated exploration of multi-principal element alloys with solid solution phases , 2015, Nature Communications.

[30]  P. Liaw,et al.  Deviation from high-entropy configurations in the atomic distributions of a multi-principal-element alloy , 2015, Nature Communications.

[31]  R. Ritchie,et al.  A fracture-resistant high-entropy alloy for cryogenic applications , 2014, Science.

[32]  M. Feuerbacher,et al.  Hexagonal High-entropy Alloys , 2014, 1408.0100.

[33]  Wei Zhang,et al.  High-Entropy Alloys with a Hexagonal Close-Packed Structure Designed by Equi-Atomic Alloy Strategy and Binary Phase Diagrams , 2014 .

[34]  K. Dahmen,et al.  Microstructures and properties of high-entropy alloys , 2014 .

[35]  Zhi Tang,et al.  Alloying and Processing Effects on the Aqueous Corrosion Behavior of High-Entropy Alloys , 2014, Entropy.

[36]  David E. Alman,et al.  Searching for Next Single-Phase High-Entropy Alloy Compositions , 2013, Entropy.

[37]  J. Crum,et al.  Epsilon metal waste form for immobilization of noble metals from used nuclear fuel , 2013 .

[38]  G. Eggeler,et al.  The influences of temperature and microstructure on the tensile properties of a CoCrFeMnNi high-entropy alloy , 2013 .

[39]  Jien-Wei Yeh,et al.  Fatigue behavior of Al0.5CoCrCuFeNi high entropy alloys , 2012 .

[40]  Yong Zhang,et al.  Prediction of high-entropy stabilized solid-solution in multi-component alloys , 2012 .

[41]  J. Yeh,et al.  Microstructure and wear behavior of AlxCo1.5CrFeNi1.5Tiy high-entropy alloys , 2011 .

[42]  C. Liu,et al.  Effect of valence electron concentration on stability of fcc or bcc phase in high entropy alloys , 2011 .

[43]  T. B. Massalski Comments Concerning Some Features of Phase Diagrams and Phase Transformations , 2010 .

[44]  Rodney C. Ewing,et al.  The fate of the epsilon phase (Mo-Ru-Pd-Tc-Rh) in the UO2 of the Oklo natural fission reactors , 2006 .

[45]  Akira Takeuchi,et al.  Classification of Bulk Metallic Glasses by Atomic Size Difference, Heat of Mixing and Period of Constituent Elements and Its Application to Characterization of the Main Alloying Element , 2005 .

[46]  B. Cantor,et al.  Microstructural development in equiatomic multicomponent alloys , 2004 .

[47]  T. Shun,et al.  Nanostructured High‐Entropy Alloys with Multiple Principal Elements: Novel Alloy Design Concepts and Outcomes , 2004 .

[48]  H. Kleykamp Constitution and thermodynamics of the Mo-Ru, Mo-Pd, Ru-Pd and Mo-Ru-Pd systems , 1989 .

[49]  T. Matsui,et al.  Chemical state, phases and vapor pressures of fission-produced noble metals in oxide fuel , 1988 .

[50]  H. Kleykamp,et al.  The chemical state of the fission products in oxide fuels , 1985 .

[51]  H. Kleykamp,et al.  Composition and structure of fission product precipitates in irradiated oxide fuels: Correlation with phase studies in the Mo-Ru-Rh-Pd and BaO-UO2-ZrO2-MoO2 Systems , 1985 .

[52]  F. L. Brown,et al.  Analysis of fission product ingots formed in uranium-plutonium oxide irradiated in EBR-II☆ , 1970 .

[53]  R. Sharpe,et al.  Metallic fission-product inclusions in irradiated oxide fuels , 1968 .

[54]  D. Cui,et al.  Characterization of alloy particles extracted from spent nuclear fuel , 2012 .

[55]  D. Cui,et al.  On Mo-Ru-Tc-Pd-Rh-Te alloy particles extracted from spent fuel and their leaching behavior under Ar and H2 atmospheres , 2004 .

[56]  H. Matzke,et al.  MICROSTRUCTURAL FEATURES OF SIMFUEL : SIMULATED HIGH-BURNUP UO2-BASED NUCLEAR FUEL , 1991 .