Phase-field modeling of diffusional phase behaviors of solid surfaces: A case study of phase-separating LiXFePO4 electrode particles
Abstract
In this paper, we present a comprehensive phase-field model for simulating diffusion-mediated kinetic phase behaviors near the surface of a solid particle. The model incorporates elastic inhomogeneity and anisotropy, diffusion mobility anisotropy, interfacial energy anisotropy, and Cahn–Hilliard diffusion kinetics. The free energy density function is formulated based on the regular solution model taking into account the possible solute-surface interaction near the surface. The coherency strain energy is computed using the Fourier-spectral iterative-perturbation method due to the strong elastic inhomogeneity with a zero surface traction boundary condition. Employing a phase-separating LiXFePO4 electrode particle for Li-ion batteries as a model system, we perform parametric three-dimensional computer simulations. The model permits the observation of surface phase behaviors that are different from the bulk counterpart. For instance, it reproduces the theoretically well-established surface modes of spinodal decomposition of an unstable solid solution: the surface mode of coherent spinodal decomposition and the surface-directed spinodal decomposition mode. We systematically investigate the influences of major factors on the kinetic surface phase behaviors during the diffusional process. Finally, our simulation study provides insights for tailoring the internal phase microstructure of a particle by controlling the surface phase morphology.
- Authors:
-
- Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States). Materials Science Division
- Pennsylvania State Univ., University Park, PA (United States). Dept. of Materials Science and Engineering
- Publication Date:
- Research Org.:
- Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States); Pennsylvania State Univ., University Park, PA (United States)
- Sponsoring Org.:
- USDOE; LLNL Laboratory Directed Research and Development (LDRD) Program; National Science Foundation (NSF)
- OSTI Identifier:
- 1251071
- Alternate Identifier(s):
- OSTI ID: 1250075
- Report Number(s):
- LLNL-JRNL-665469
Journal ID: ISSN 0927-0256
- Grant/Contract Number:
- AC52-07NA27344; CMMI-1235092
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Computational Materials Science
- Additional Journal Information:
- Journal Volume: 108; Journal Issue: B; Journal ID: ISSN 0927-0256
- Publisher:
- Elsevier
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; 25 ENERGY STORAGE; phase-field model; solid surface; phase behavior; electrode particle
Citation Formats
Heo, Tae Wook, Chen, Long-Qing, and Wood, Brandon C. Phase-field modeling of diffusional phase behaviors of solid surfaces: A case study of phase-separating LiXFePO4 electrode particles. United States: N. p., 2015.
Web. doi:10.1016/j.commatsci.2015.03.020.
Heo, Tae Wook, Chen, Long-Qing, & Wood, Brandon C. Phase-field modeling of diffusional phase behaviors of solid surfaces: A case study of phase-separating LiXFePO4 electrode particles. United States. https://doi.org/10.1016/j.commatsci.2015.03.020
Heo, Tae Wook, Chen, Long-Qing, and Wood, Brandon C. Wed .
"Phase-field modeling of diffusional phase behaviors of solid surfaces: A case study of phase-separating LiXFePO4 electrode particles". United States. https://doi.org/10.1016/j.commatsci.2015.03.020. https://www.osti.gov/servlets/purl/1251071.
@article{osti_1251071,
title = {Phase-field modeling of diffusional phase behaviors of solid surfaces: A case study of phase-separating LiXFePO4 electrode particles},
author = {Heo, Tae Wook and Chen, Long-Qing and Wood, Brandon C.},
abstractNote = {In this paper, we present a comprehensive phase-field model for simulating diffusion-mediated kinetic phase behaviors near the surface of a solid particle. The model incorporates elastic inhomogeneity and anisotropy, diffusion mobility anisotropy, interfacial energy anisotropy, and Cahn–Hilliard diffusion kinetics. The free energy density function is formulated based on the regular solution model taking into account the possible solute-surface interaction near the surface. The coherency strain energy is computed using the Fourier-spectral iterative-perturbation method due to the strong elastic inhomogeneity with a zero surface traction boundary condition. Employing a phase-separating LiXFePO4 electrode particle for Li-ion batteries as a model system, we perform parametric three-dimensional computer simulations. The model permits the observation of surface phase behaviors that are different from the bulk counterpart. For instance, it reproduces the theoretically well-established surface modes of spinodal decomposition of an unstable solid solution: the surface mode of coherent spinodal decomposition and the surface-directed spinodal decomposition mode. We systematically investigate the influences of major factors on the kinetic surface phase behaviors during the diffusional process. Finally, our simulation study provides insights for tailoring the internal phase microstructure of a particle by controlling the surface phase morphology.},
doi = {10.1016/j.commatsci.2015.03.020},
journal = {Computational Materials Science},
number = B,
volume = 108,
place = {United States},
year = {Wed Apr 08 00:00:00 EDT 2015},
month = {Wed Apr 08 00:00:00 EDT 2015}
}
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Works referencing / citing this record:
A mechanism of defect-enhanced phase transformation kinetics in lithium iron phosphate olivine
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