A model for multicomponent diffusion in oxide melts

Sun Yong Kwon; Reghan J. Hill; In Ho Jung

doi:10.1016/j.calphad.2020.102246

A model for multicomponent diffusion in oxide melts

Sun Yong Kwon
, Reghan J. Hill
, In Ho Jung

Research output: Contribution to journal › Article › peer-review

3 Scopus citations

Abstract

A general flux equation for multicomponent diffusion in oxide melts is presented. An explicit method was developed to calculate the gradients of single-ion activities from those of oxides with the constraints of local equilibrium and electroneutrality. This resolves ambiguity in quantifying the thermochemical driving force for ionic diffusion. A model equation for multicomponent ionic diffusion was derived within the framework of non-equilibrium thermodynamics by de Groot and Mazur. The proposed model takes empirically measurable quantities as input variables, so the diffusion calculations are consistent with thermochemical data, as furnished by the CALPHAD (CALculation of PHAse Diagrams) method, as well as ionic mobility measurements. Although the model is derived for oxides, it can be applied to diffusion in other concentrated liquid electrolytes, such as chloride and fluoride melts. Formulas for multicomponent ionic diffusion in various reference frames are presented with respect to mole fraction.

Original language	English
Article number	102246
Journal	Calphad: Computer Coupling of Phase Diagrams and Thermochemistry
Volume	72
DOIs	https://doi.org/10.1016/j.calphad.2020.102246
State	Published - Mar 2021
Externally published	Yes

Funding

This research was possible through funding by a collaborative research and development (CRD) grant from the Natural Sciences and Engineering Research Council (NSERC) of Canada in collaboration with Almatis, Doosan Heavy Industry and Construction, Elkem, Hyundai Steel, Imerys, JFE Steel, Nippon Steel and Sumitomo MetalsCorp. Nucor Steel, Posco, RHI Magnesita, RioTinto Iron and Titanium, RIST, SeAh Besteel, Shott AG, Tata Steel Europe, and Voestalpine. This work was also supported by the National Research Foundation of Korea (NRF) grant funded by the Korean government (MSIT) (No. NRF-2020R1A5A6017701). This research was possible through funding by a collaborative research and development (CRD) grant from the Natural Sciences and Engineering Research Council (NSERC) of Canada in collaboration with Almatis, Doosan Heavy Industry and Construction, Elkem, Hyundai Steel, Imerys, JFE Steel, Nippon Steel and Sumitomo MetalsCorp., Nucor Steel, Posco, RHI Magnesita, RioTinto Iron and Titanium, RIST, SeAh Besteel, Shott AG, Tata Steel Europe, and Voestalpine. This work was also supported by the National Research Foundation of Korea (NRF) grant funded by the Korean government (MSIT) (No. NRF-2020R1A5A6017701 ).

Keywords

Electrolytes
Entropy production
Multicomponent diffusion
Non-equilibrium thermodynamics
Oxide melts
Single-ion activity

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10.1016/j.calphad.2020.102246

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title = "A model for multicomponent diffusion in oxide melts",

abstract = "A general flux equation for multicomponent diffusion in oxide melts is presented. An explicit method was developed to calculate the gradients of single-ion activities from those of oxides with the constraints of local equilibrium and electroneutrality. This resolves ambiguity in quantifying the thermochemical driving force for ionic diffusion. A model equation for multicomponent ionic diffusion was derived within the framework of non-equilibrium thermodynamics by de Groot and Mazur. The proposed model takes empirically measurable quantities as input variables, so the diffusion calculations are consistent with thermochemical data, as furnished by the CALPHAD (CALculation of PHAse Diagrams) method, as well as ionic mobility measurements. Although the model is derived for oxides, it can be applied to diffusion in other concentrated liquid electrolytes, such as chloride and fluoride melts. Formulas for multicomponent ionic diffusion in various reference frames are presented with respect to mole fraction.",

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doi = "10.1016/j.calphad.2020.102246",

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T1 - A model for multicomponent diffusion in oxide melts

AU - Kwon, Sun Yong

AU - Hill, Reghan J.

AU - Jung, In Ho

PY - 2021/3

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N2 - A general flux equation for multicomponent diffusion in oxide melts is presented. An explicit method was developed to calculate the gradients of single-ion activities from those of oxides with the constraints of local equilibrium and electroneutrality. This resolves ambiguity in quantifying the thermochemical driving force for ionic diffusion. A model equation for multicomponent ionic diffusion was derived within the framework of non-equilibrium thermodynamics by de Groot and Mazur. The proposed model takes empirically measurable quantities as input variables, so the diffusion calculations are consistent with thermochemical data, as furnished by the CALPHAD (CALculation of PHAse Diagrams) method, as well as ionic mobility measurements. Although the model is derived for oxides, it can be applied to diffusion in other concentrated liquid electrolytes, such as chloride and fluoride melts. Formulas for multicomponent ionic diffusion in various reference frames are presented with respect to mole fraction.

AB - A general flux equation for multicomponent diffusion in oxide melts is presented. An explicit method was developed to calculate the gradients of single-ion activities from those of oxides with the constraints of local equilibrium and electroneutrality. This resolves ambiguity in quantifying the thermochemical driving force for ionic diffusion. A model equation for multicomponent ionic diffusion was derived within the framework of non-equilibrium thermodynamics by de Groot and Mazur. The proposed model takes empirically measurable quantities as input variables, so the diffusion calculations are consistent with thermochemical data, as furnished by the CALPHAD (CALculation of PHAse Diagrams) method, as well as ionic mobility measurements. Although the model is derived for oxides, it can be applied to diffusion in other concentrated liquid electrolytes, such as chloride and fluoride melts. Formulas for multicomponent ionic diffusion in various reference frames are presented with respect to mole fraction.

KW - Electrolytes

KW - Entropy production

KW - Multicomponent diffusion

KW - Non-equilibrium thermodynamics

KW - Oxide melts

KW - Single-ion activity

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DO - 10.1016/j.calphad.2020.102246

M3 - Article

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JF - Calphad: Computer Coupling of Phase Diagrams and Thermochemistry

M1 - 102246

ER -

A model for multicomponent diffusion in oxide melts

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