Atomic mechanism of lithium dendrite penetration in solid electrolytes
Abstract Lithium dendrite penetration through ceramic electrolytes is known to result in mechanical failure and short circuits, which has impeded the commercialization of all-solid-state lithium anode batteries. However, the underlying mechanism still remains under debate, due in part to a lack of i...
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Nature Portfolio
2025-02-01
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| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-025-57259-x |
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| author | Bowen Zhang Botao Yuan Xin Yan Xiao Han Jiawei Zhang Huifeng Tan Changuo Wang Pengfei Yan Huajian Gao Yuanpeng Liu |
| author_facet | Bowen Zhang Botao Yuan Xin Yan Xiao Han Jiawei Zhang Huifeng Tan Changuo Wang Pengfei Yan Huajian Gao Yuanpeng Liu |
| author_sort | Bowen Zhang |
| collection | DOAJ |
| description | Abstract Lithium dendrite penetration through ceramic electrolytes is known to result in mechanical failure and short circuits, which has impeded the commercialization of all-solid-state lithium anode batteries. However, the underlying mechanism still remains under debate, due in part to a lack of in situ atomic-level observations of the dendrite penetration process. Here, we employ molecular dynamics simulations to reproduce the dynamic process of dendrite nucleation and penetration. Our findings reveal that dynamically generated lithium depositions lead to a continuous accumulation of internal stress, culminating in fracture of the solid electrolyte at dendrite tips. We demonstrate that the classical Griffith theory remains effective in assessing this fracture mode, but it is necessary to consider the electrochemical impact of local lithium ion concentration on the fracture toughness. Additionally, in polycrystalline solid electrolytes, we observe that dendrite nuclei within grains typically deflect towards and propagate along grain boundaries. Simulations and experimental evidence both identify that dendrite induced fractures at grain boundaries exhibit a mixed Mode I and Mode II pattern, contingent on their fracture toughness and the angle between dendrites and grain boundaries. These insights deepen our understanding of dendrite penetration mechanisms and may offer valuable guidance for improving the performance of solid electrolytes. |
| format | Article |
| id | doaj-art-4836b1c7b7f64be9934d743d758fca79 |
| institution | DOAJ |
| issn | 2041-1723 |
| language | English |
| publishDate | 2025-02-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Nature Communications |
| spelling | doaj-art-4836b1c7b7f64be9934d743d758fca792025-08-20T03:04:07ZengNature PortfolioNature Communications2041-17232025-02-0116111310.1038/s41467-025-57259-xAtomic mechanism of lithium dendrite penetration in solid electrolytesBowen Zhang0Botao Yuan1Xin Yan2Xiao Han3Jiawei Zhang4Huifeng Tan5Changuo Wang6Pengfei Yan7Huajian Gao8Yuanpeng Liu9Center for Composite Materials, Harbin Institute of TechnologyCenter for Composite Materials, Harbin Institute of TechnologySchool of Mechanical Engineering and Automation, Beihang UniversityBeijing Key Laboratory of Microstructure and Property of Solids, Faculty of Materials and Manufacturing, Beijing University of TechnologyCenter for Composite Materials, Harbin Institute of TechnologyCenter for Composite Materials, Harbin Institute of TechnologyCenter for Composite Materials, Harbin Institute of TechnologyBeijing Key Laboratory of Microstructure and Property of Solids, Faculty of Materials and Manufacturing, Beijing University of TechnologySchool of Mechanical and Aerospace Engineering, Nanyang Technological UniversityCenter for Composite Materials, Harbin Institute of TechnologyAbstract Lithium dendrite penetration through ceramic electrolytes is known to result in mechanical failure and short circuits, which has impeded the commercialization of all-solid-state lithium anode batteries. However, the underlying mechanism still remains under debate, due in part to a lack of in situ atomic-level observations of the dendrite penetration process. Here, we employ molecular dynamics simulations to reproduce the dynamic process of dendrite nucleation and penetration. Our findings reveal that dynamically generated lithium depositions lead to a continuous accumulation of internal stress, culminating in fracture of the solid electrolyte at dendrite tips. We demonstrate that the classical Griffith theory remains effective in assessing this fracture mode, but it is necessary to consider the electrochemical impact of local lithium ion concentration on the fracture toughness. Additionally, in polycrystalline solid electrolytes, we observe that dendrite nuclei within grains typically deflect towards and propagate along grain boundaries. Simulations and experimental evidence both identify that dendrite induced fractures at grain boundaries exhibit a mixed Mode I and Mode II pattern, contingent on their fracture toughness and the angle between dendrites and grain boundaries. These insights deepen our understanding of dendrite penetration mechanisms and may offer valuable guidance for improving the performance of solid electrolytes.https://doi.org/10.1038/s41467-025-57259-x |
| spellingShingle | Bowen Zhang Botao Yuan Xin Yan Xiao Han Jiawei Zhang Huifeng Tan Changuo Wang Pengfei Yan Huajian Gao Yuanpeng Liu Atomic mechanism of lithium dendrite penetration in solid electrolytes Nature Communications |
| title | Atomic mechanism of lithium dendrite penetration in solid electrolytes |
| title_full | Atomic mechanism of lithium dendrite penetration in solid electrolytes |
| title_fullStr | Atomic mechanism of lithium dendrite penetration in solid electrolytes |
| title_full_unstemmed | Atomic mechanism of lithium dendrite penetration in solid electrolytes |
| title_short | Atomic mechanism of lithium dendrite penetration in solid electrolytes |
| title_sort | atomic mechanism of lithium dendrite penetration in solid electrolytes |
| url | https://doi.org/10.1038/s41467-025-57259-x |
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