Phase-Field Computational Framework for Addressing Challenges in Solid-State Batteries
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-...
| Main Authors: | , , , , , , , , , |
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| Format: | Article |
| Language: | English |
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American Physical Society
2024
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| Online Access: | https://hdl.handle.net/1721.1/157521 |
| _version_ | 1824458451499089920 |
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| author | Schwietert, Tammo K Ombrini, Pierfrancesco Ootes, Laura S Oostrum, Leon Azizi, Victor Cogswell, Daniel Zhu, Juner Bazant, Martin Z Wagemaker, Marnix Vasileiadis, Alexandros |
| author2 | Massachusetts Institute of Technology. Department of Chemical Engineering |
| author_facet | Massachusetts Institute of Technology. Department of Chemical Engineering Schwietert, Tammo K Ombrini, Pierfrancesco Ootes, Laura S Oostrum, Leon Azizi, Victor Cogswell, Daniel Zhu, Juner Bazant, Martin Z Wagemaker, Marnix Vasileiadis, Alexandros |
| author_sort | Schwietert, Tammo K |
| collection | MIT |
| description | 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. |
| first_indexed | 2025-02-19T04:26:06Z |
| format | Article |
| id | mit-1721.1/157521 |
| institution | Massachusetts Institute of Technology |
| language | English |
| last_indexed | 2025-02-19T04:26:06Z |
| publishDate | 2024 |
| publisher | American Physical Society |
| record_format | dspace |
| spelling | mit-1721.1/1575212025-01-08T04:13:36Z Phase-Field Computational Framework for Addressing Challenges in Solid-State Batteries Schwietert, Tammo K Ombrini, Pierfrancesco Ootes, Laura S Oostrum, Leon Azizi, Victor Cogswell, Daniel Zhu, Juner Bazant, Martin Z Wagemaker, Marnix Vasileiadis, Alexandros Massachusetts Institute of Technology. Department of Chemical Engineering Massachusetts Institute of Technology. Department of Mathematics 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. 2024-11-08T20:14:39Z 2024-11-08T20:14:39Z 2023 2024-11-08T20:09:31Z Article http://purl.org/eprint/type/JournalArticle https://hdl.handle.net/1721.1/157521 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). en 10.1103/prxenergy.2.033014 PRX Energy Creative Commons Attribution https://creativecommons.org/licenses/by/4.0/ application/pdf American Physical Society American Physical Society |
| spellingShingle | Schwietert, Tammo K Ombrini, Pierfrancesco Ootes, Laura S Oostrum, Leon Azizi, Victor Cogswell, Daniel Zhu, Juner Bazant, Martin Z Wagemaker, Marnix Vasileiadis, Alexandros Phase-Field Computational Framework for Addressing Challenges in Solid-State Batteries |
| title | Phase-Field Computational Framework for Addressing Challenges in Solid-State Batteries |
| title_full | Phase-Field Computational Framework for Addressing Challenges in Solid-State Batteries |
| title_fullStr | Phase-Field Computational Framework for Addressing Challenges in Solid-State Batteries |
| title_full_unstemmed | Phase-Field Computational Framework for Addressing Challenges in Solid-State Batteries |
| title_short | Phase-Field Computational Framework for Addressing Challenges in Solid-State Batteries |
| title_sort | phase field computational framework for addressing challenges in solid state batteries |
| url | https://hdl.handle.net/1721.1/157521 |
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