A self-healing plastic ceramic electrolyte by an aprotic dynamic polymer network for lithium metal batteries
Abstract Oxide ceramic electrolytes (OCEs) have great potential for solid-state lithium metal (Li0) battery applications because, in theory, their high elastic modulus provides better resistance to Li0 dendrite growth. However, in practice, OCEs can hardly survive critical current densities higher t...
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Nature Portfolio
2024-11-01
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| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-024-53869-z |
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| author | Yubin He Chunyang Wang Rui Zhang Peichao Zou Zhouyi Chen Seong-Min Bak Stephen E. Trask Yonghua Du Ruoqian Lin Enyuan Hu Huolin L. Xin |
| author_facet | Yubin He Chunyang Wang Rui Zhang Peichao Zou Zhouyi Chen Seong-Min Bak Stephen E. Trask Yonghua Du Ruoqian Lin Enyuan Hu Huolin L. Xin |
| author_sort | Yubin He |
| collection | DOAJ |
| description | Abstract Oxide ceramic electrolytes (OCEs) have great potential for solid-state lithium metal (Li0) battery applications because, in theory, their high elastic modulus provides better resistance to Li0 dendrite growth. However, in practice, OCEs can hardly survive critical current densities higher than 1 mA/cm2. Key issues that contribute to the breakdown of OCEs include Li0 penetration promoted by grain boundaries (GBs), uncontrolled side reactions at electrode-OCE interfaces, and, equally importantly, defects evolution (e.g., void growth and crack propagation) that leads to local current concentration and mechanical failure inside and on OCEs. Here, taking advantage of a dynamically crosslinked aprotic polymer with non-covalent –CH3⋯CF3 bonds, we developed a plastic ceramic electrolyte (PCE) by hybridizing the polymer framework with ionically conductive ceramics. Using in-situ synchrotron X-ray technique and Cryogenic transmission electron microscopy (Cryo-TEM), we uncover that the PCE exhibits self-healing/repairing capability through a two-step dynamic defects removal mechanism. This significantly suppresses the generation of hotspots for Li0 penetration and chemomechanical degradations, resulting in durability beyond 2000 hours in Li0-Li0 cells at 1 mA/cm2. Furthermore, by introducing a polyacrylate buffer layer between PCE and Li0-anode, long cycle life >3600 cycles was achieved when paired with a 4.2 V zero-strain cathode, all under near-zero stack pressure. |
| format | Article |
| id | doaj-art-e6ffcc703e8441d6a1dfd7bd26652a3e |
| institution | OA Journals |
| issn | 2041-1723 |
| language | English |
| publishDate | 2024-11-01 |
| publisher | Nature Portfolio |
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| series | Nature Communications |
| spelling | doaj-art-e6ffcc703e8441d6a1dfd7bd26652a3e2025-08-20T02:22:24ZengNature PortfolioNature Communications2041-17232024-11-0115111310.1038/s41467-024-53869-zA self-healing plastic ceramic electrolyte by an aprotic dynamic polymer network for lithium metal batteriesYubin He0Chunyang Wang1Rui Zhang2Peichao Zou3Zhouyi Chen4Seong-Min Bak5Stephen E. Trask6Yonghua Du7Ruoqian Lin8Enyuan Hu9Huolin L. Xin10Department of Physics and Astronomy, University of CaliforniaDepartment of Physics and Astronomy, University of CaliforniaDepartment of Physics and Astronomy, University of CaliforniaDepartment of Physics and Astronomy, University of CaliforniaDepartment of Physics and Astronomy, University of CaliforniaNational Synchrotron Light Source II, Brookhaven National LaboratoryCell Analysis, Modeling, and Prototyping Facility, Argonne National LaboratoryNational Synchrotron Light Source II, Brookhaven National LaboratoryDepartment of Mechanical Engineering, University of CaliforniaChemistry Division, Brookhaven National LaboratoryDepartment of Physics and Astronomy, University of CaliforniaAbstract Oxide ceramic electrolytes (OCEs) have great potential for solid-state lithium metal (Li0) battery applications because, in theory, their high elastic modulus provides better resistance to Li0 dendrite growth. However, in practice, OCEs can hardly survive critical current densities higher than 1 mA/cm2. Key issues that contribute to the breakdown of OCEs include Li0 penetration promoted by grain boundaries (GBs), uncontrolled side reactions at electrode-OCE interfaces, and, equally importantly, defects evolution (e.g., void growth and crack propagation) that leads to local current concentration and mechanical failure inside and on OCEs. Here, taking advantage of a dynamically crosslinked aprotic polymer with non-covalent –CH3⋯CF3 bonds, we developed a plastic ceramic electrolyte (PCE) by hybridizing the polymer framework with ionically conductive ceramics. Using in-situ synchrotron X-ray technique and Cryogenic transmission electron microscopy (Cryo-TEM), we uncover that the PCE exhibits self-healing/repairing capability through a two-step dynamic defects removal mechanism. This significantly suppresses the generation of hotspots for Li0 penetration and chemomechanical degradations, resulting in durability beyond 2000 hours in Li0-Li0 cells at 1 mA/cm2. Furthermore, by introducing a polyacrylate buffer layer between PCE and Li0-anode, long cycle life >3600 cycles was achieved when paired with a 4.2 V zero-strain cathode, all under near-zero stack pressure.https://doi.org/10.1038/s41467-024-53869-z |
| spellingShingle | Yubin He Chunyang Wang Rui Zhang Peichao Zou Zhouyi Chen Seong-Min Bak Stephen E. Trask Yonghua Du Ruoqian Lin Enyuan Hu Huolin L. Xin A self-healing plastic ceramic electrolyte by an aprotic dynamic polymer network for lithium metal batteries Nature Communications |
| title | A self-healing plastic ceramic electrolyte by an aprotic dynamic polymer network for lithium metal batteries |
| title_full | A self-healing plastic ceramic electrolyte by an aprotic dynamic polymer network for lithium metal batteries |
| title_fullStr | A self-healing plastic ceramic electrolyte by an aprotic dynamic polymer network for lithium metal batteries |
| title_full_unstemmed | A self-healing plastic ceramic electrolyte by an aprotic dynamic polymer network for lithium metal batteries |
| title_short | A self-healing plastic ceramic electrolyte by an aprotic dynamic polymer network for lithium metal batteries |
| title_sort | self healing plastic ceramic electrolyte by an aprotic dynamic polymer network for lithium metal batteries |
| url | https://doi.org/10.1038/s41467-024-53869-z |
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