Phase Stability for the Pd-Si System. First-Principles, Experiments, and Solution-Based Modeling

Zhou, S. H.; Huo, Y.; Napolitano, Ralph E.

doi:10.1007/s11661-015-3206-8

Title: Phase Stability for the Pd-Si System. First-Principles, Experiments, and Solution-Based Modeling

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Abstract

Relative stabilities of the compounds in the binary Pd-Si system were assessed using first-principles calculations and experimental methods. Calculations of lattice parameters and enthalpy of formation indicate that Pd₅Si-μ, Pd₉Si₂-α, Pd₃ Si-β, Pd₂ Si-γ, and PdSi-δ are the stable phases at 0 K (-273 °C). X-ray diffraction analyses (XRD) and electron probe microanalysis (EPMA) of the as-solidified and heat-treated samples support the computational findings, except that the PdSi-δ phase was not observed at low temperature. Considering both experimental data and first-principles results, the compounds Pd ₅ Si-μ, Pd₉ Si₂-α, Pd₃Si-β, and Pd₂Si-γ are treated as stable phases down to 0 K (-273 °C), while the PdSi-δ is treated as being stable over a limited range, exhibiting a lower bound. Using these findings, a comprehensive solution-based thermodynamic model is formulated for the Pd-Si system, permitting phase diagram calculation. Moreover, the liquid phase is described using a three-species association model and other phases are treated as solid solutions, where a random substitutional model is adopted for Pd-fcc and Si-dia, and a two-sublattice model is employed for Pd₅Si-μ, Pd₉Si₂-α, Pd₃Si-β, Pd₂Si-γ, and PdSi-δ. Model parameters are fitted using available experimental data and first-principles data, and the resulting phase diagram is reported over themore » full range of compositions.« less

Authors:

Zhou, S. H. ^[1]; Huo, Y. ^[2]; Napolitano, Ralph E. ^[2]

Ames Lab., Ames, IA (United States)
Iowa State Univ., Ames, IA (United States)

Publication Date:: Thu Nov 05 00:00:00 EST 2015

Research Org.:: Ames Lab., Ames, IA (United States)

Sponsoring Org.:: USDOE

OSTI Identifier:: 1234457

Report Number(s):: IS-J 8863
Journal ID: ISSN 1073-5623; PII: 3206

Grant/Contract Number:: AC02-07CH11358

Resource Type:: Accepted Manuscript

Journal Name:: Metallurgical and Materials Transactions. A, Physical Metallurgy and Materials Science

Additional Journal Information:: Journal Volume: 47; Journal Issue: 1; Journal ID: ISSN 1073-5623

Publisher:: ASM International

Country of Publication:: United States

Language:: English

Subject:: 36 MATERIALS SCIENCE

Citation Formats


                    Zhou, S. H., Huo, Y., and Napolitano, Ralph E. Phase Stability for the Pd-Si System. First-Principles, Experiments, and Solution-Based Modeling.  United States: N. p., 2015. 
Web.  doi:10.1007/s11661-015-3206-8.

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                    Zhou, S. H., Huo, Y., & Napolitano, Ralph E. Phase Stability for the Pd-Si System. First-Principles, Experiments, and Solution-Based Modeling.  United States.  https://doi.org/10.1007/s11661-015-3206-8

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                    Zhou, S. H., Huo, Y., and Napolitano, Ralph E. Thu .  
"Phase Stability for the Pd-Si System. First-Principles, Experiments, and Solution-Based Modeling".  United States.  https://doi.org/10.1007/s11661-015-3206-8.  https://www.osti.gov/servlets/purl/1234457.

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@article{osti_1234457,

  title        = {Phase Stability for the Pd-Si System. First-Principles, Experiments, and Solution-Based Modeling},

  author       = {Zhou, S. H. and Huo, Y. and Napolitano, Ralph E.},

  abstractNote = {Relative stabilities of the compounds in the binary Pd-Si system were assessed using first-principles calculations and experimental methods. Calculations of lattice parameters and enthalpy of formation indicate that Pd5Si-μ, Pd9Si2-α, Pd3 Si-β, Pd2 Si-γ, and PdSi-δ are the stable phases at 0 K (-273 °C). X-ray diffraction analyses (XRD) and electron probe microanalysis (EPMA) of the as-solidified and heat-treated samples support the computational findings, except that the PdSi-δ phase was not observed at low temperature. Considering both experimental data and first-principles results, the compounds Pd 5 Si-μ, Pd9 Si2-α, Pd3Si-β, and Pd2Si-γ are treated as stable phases down to 0 K (-273 °C), while the PdSi-δ is treated as being stable over a limited range, exhibiting a lower bound. Using these findings, a comprehensive solution-based thermodynamic model is formulated for the Pd-Si system, permitting phase diagram calculation. Moreover, the liquid phase is described using a three-species association model and other phases are treated as solid solutions, where a random substitutional model is adopted for Pd-fcc and Si-dia, and a two-sublattice model is employed for Pd5Si-μ, Pd9Si2-α, Pd3Si-β, Pd2Si-γ, and PdSi-δ. Model parameters are fitted using available experimental data and first-principles data, and the resulting phase diagram is reported over the full range of compositions.},

  doi          = {10.1007/s11661-015-3206-8},

  journal      = {Metallurgical and Materials Transactions. A, Physical Metallurgy and Materials Science},

  number       = 1,

  volume       = 47,

  place        = {United States},

  year         = {Thu Nov 05 00:00:00 EST 2015},

  month        = {Thu Nov 05 00:00:00 EST 2015}

}

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