Phase-Field Computational Framework for Addressing Challenges in Solid-State Batteries
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PRXEnergy.2.033014.pdf
Description
Published version
Size
3.68 MB
Format
Adobe PDF
Checksum (MD5)
35d96423511f3709650b61ca25c9db52
Author(s)
Schwietert, Tammo K
Ombrini, Pierfrancesco
Ootes, Laura S
Oostrum, Leon
Azizi, Victor
Cogswell, Daniel
Zhu, Juner
Bazant, Martin Z
Wagemaker, Marnix
Vasileiadis, Alexandros
Date Issued
2023
Journal
PRX Energy
Publisher
American Physical Society
Citation
Schwietert, Tammo K, Ombrini, Pierfrancesco, Ootes, Laura S, Oostrum, Leon, Azizi, Victor et al. 2023. "Phase-Field Computational Framework for Addressing Challenges in Solid-State Batteries." PRX Energy, 2 (3).
Version
Final published version
Abstract
All-solid-state batteries are attracting increasing interest due to their higher promised energy densities without the use of flammable liquid electrolytes. Two main challenges for solid-state batteries are contact loss and interphase formation; these play a central role in the quality of the solid-electrolyte–electrode interfaces. Here, we present a modular phase-field modeling framework that is generally applicable to solid-state batteries with different electrodes and corresponding microstructures. The model is based on multiphase porous electrode theory, where Li-ion diffusion in solid electrolytes and electrode materials is integrated through a regular solution free energy functional. Modules for contact loss and diffusive interlayers, able to capture solid-solid and solid-liquid interfaces such as solid-electrolyte interphase formation and coatings, are also implemented, providing numerous modeling options for a comprehensive understanding of electrochemical systems. A thorough comparison between the solid-state and conventional liquid-electrolyte models for phase-separating electrodes reveals the optimal conditions and bottlenecks of solid-state diffusion and failure mechanisms. The predictions underline contact loss and interphase formation as the crucial mesoscopic morphological characteristics of solid-state systems, setting the basis for in-depth understanding and optimized performance in all-solid-state batteries.
MIT Department
Massachusetts Institute of Technology. Department of Chemical Engineering
Massachusetts Institute of Technology. Department of Mathematics
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DOI of Published Version
https://doi.org/10.1103/prxenergy.2.033014
