Progressive growth of the solid–electrolyte interphase towards the Si anode interior causes capacity fading
The solid–electrolyte interphase (SEI), a layer formed on the electrode surface, is essential for electrochemical reactions in batteries and critically governs the battery stability. Active materials, especially those with extremely high energy density, such as silicon (Si), often inevitably undergo...
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| Published in | Nature nanotechnology Vol. 16; no. 10; pp. 1113 - 1120 |
|---|---|
| Main Authors | , , , , , , , , , , , , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
London
Nature Publishing Group UK
01.10.2021
Nature Publishing Group |
| Subjects | |
| Online Access | Get full text |
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| Abstract | The solid–electrolyte interphase (SEI), a layer formed on the electrode surface, is essential for electrochemical reactions in batteries and critically governs the battery stability. Active materials, especially those with extremely high energy density, such as silicon (Si), often inevitably undergo a large volume swing upon ion insertion and extraction, raising a critical question as to how the SEI interactively responds to and evolves with the material and consequently controls the cycling stability of the battery. Here, by integrating sensitive elemental tomography, an advanced algorithm and cryogenic scanning transmission electron microscopy, we unveil, in three dimensions, a correlated structural and chemical evolution of Si and SEI. Corroborated with a chemomechanical model, we demonstrate progressive electrolyte permeation and SEI growth along the percolation channel of the nanovoids due to vacancy injection and condensation during the delithiation process. Consequently, the Si–SEI spatial configuration evolves from the classic ‘core–shell’ structure in the first few cycles to a ‘plum-pudding’ structure following extended cycling, featuring the engulfing of Si domains by the SEI, which leads to the disruption of electron conduction pathways and formation of dead Si, contributing to capacity loss. The spatially coupled interactive evolution model of SEI and active materials, in principle, applies to a broad class of high-capacity electrode materials, leading to a critical insight for remedying the fading of high-capacity electrodes.
A correlated structural and chemical evolution of silicon and the solid–electrolyte interphase was unveiled in three dimensions by integrating sensitive elemental tomography, an advanced algorithm and cryogenic scanning transmission electron microscopy. |
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| AbstractList | The solid–electrolyte interphase (SEI), a layer formed on the electrode surface, is essential for electrochemical reactions in batteries and critically governs the battery stability. Active materials, especially those with extremely high energy density, such as silicon (Si), often inevitably undergo a large volume swing upon ion insertion and extraction, raising a critical question as to how the SEI interactively responds to and evolves with the material and consequently controls the cycling stability of the battery. Here, by integrating sensitive elemental tomography, an advanced algorithm and cryogenic scanning transmission electron microscopy, we unveil, in three dimensions, a correlated structural and chemical evolution of Si and SEI. Furthermore, corroborated with a chemomechanical model, we demonstrate progressive electrolyte permeation and SEI growth along the percolation channel of the nanovoids due to vacancy injection and condensation during the delithiation process. Consequently, the Si–SEI spatial configuration evolves from the classic ‘core–shell’ structure in the first few cycles to a ‘plum-pudding’ structure following extended cycling, featuring the engulfing of Si domains by the SEI, which leads to the disruption of electron conduction pathways and formation of dead Si, contributing to capacity loss. The spatially coupled interactive evolution model of SEI and active materials, in principle, applies to a broad class of high-capacity electrode materials, leading to a critical insight for remedying the fading of high-capacity electrodes. The solid-electrolyte interphase (SEI), a layer formed on the electrode surface, is essential for electrochemical reactions in batteries and critically governs the battery stability. Active materials, especially those with extremely high energy density, such as silicon (Si), often inevitably undergo a large volume swing upon ion insertion and extraction, raising a critical question as to how the SEI interactively responds to and evolves with the material and consequently controls the cycling stability of the battery. Here, by integrating sensitive elemental tomography, an advanced algorithm and cryogenic scanning transmission electron microscopy, we unveil, in three dimensions, a correlated structural and chemical evolution of Si and SEI. Corroborated with a chemomechanical model, we demonstrate progressive electrolyte permeation and SEI growth along the percolation channel of the nanovoids due to vacancy injection and condensation during the delithiation process. Consequently, the Si-SEI spatial configuration evolves from the classic 'core-shell' structure in the first few cycles to a 'plum-pudding' structure following extended cycling, featuring the engulfing of Si domains by the SEI, which leads to the disruption of electron conduction pathways and formation of dead Si, contributing to capacity loss. The spatially coupled interactive evolution model of SEI and active materials, in principle, applies to a broad class of high-capacity electrode materials, leading to a critical insight for remedying the fading of high-capacity electrodes.The solid-electrolyte interphase (SEI), a layer formed on the electrode surface, is essential for electrochemical reactions in batteries and critically governs the battery stability. Active materials, especially those with extremely high energy density, such as silicon (Si), often inevitably undergo a large volume swing upon ion insertion and extraction, raising a critical question as to how the SEI interactively responds to and evolves with the material and consequently controls the cycling stability of the battery. Here, by integrating sensitive elemental tomography, an advanced algorithm and cryogenic scanning transmission electron microscopy, we unveil, in three dimensions, a correlated structural and chemical evolution of Si and SEI. Corroborated with a chemomechanical model, we demonstrate progressive electrolyte permeation and SEI growth along the percolation channel of the nanovoids due to vacancy injection and condensation during the delithiation process. Consequently, the Si-SEI spatial configuration evolves from the classic 'core-shell' structure in the first few cycles to a 'plum-pudding' structure following extended cycling, featuring the engulfing of Si domains by the SEI, which leads to the disruption of electron conduction pathways and formation of dead Si, contributing to capacity loss. The spatially coupled interactive evolution model of SEI and active materials, in principle, applies to a broad class of high-capacity electrode materials, leading to a critical insight for remedying the fading of high-capacity electrodes. The solid-electrolyte interphase (SEI), a layer formed on the electrode surface, is essential for electrochemical reactions in batteries and critically governs the battery stability. Active materials, especially those with extremely high energy density, such as silicon (Si), often inevitably undergo a large volume swing upon ion insertion and extraction, raising a critical question as to how the SEI interactively responds to and evolves with the material and consequently controls the cycling stability of the battery. Here, by integrating sensitive elemental tomography, an advanced algorithm and cryogenic scanning transmission electron microscopy, we unveil, in three dimensions, a correlated structural and chemical evolution of Si and SEI. Corroborated with a chemomechanical model, we demonstrate progressive electrolyte permeation and SEI growth along the percolation channel of the nanovoids due to vacancy injection and condensation during the delithiation process. Consequently, the Si-SEI spatial configuration evolves from the classic 'core-shell' structure in the first few cycles to a 'plum-pudding' structure following extended cycling, featuring the engulfing of Si domains by the SEI, which leads to the disruption of electron conduction pathways and formation of dead Si, contributing to capacity loss. The spatially coupled interactive evolution model of SEI and active materials, in principle, applies to a broad class of high-capacity electrode materials, leading to a critical insight for remedying the fading of high-capacity electrodes. The solid–electrolyte interphase (SEI), a layer formed on the electrode surface, is essential for electrochemical reactions in batteries and critically governs the battery stability. Active materials, especially those with extremely high energy density, such as silicon (Si), often inevitably undergo a large volume swing upon ion insertion and extraction, raising a critical question as to how the SEI interactively responds to and evolves with the material and consequently controls the cycling stability of the battery. Here, by integrating sensitive elemental tomography, an advanced algorithm and cryogenic scanning transmission electron microscopy, we unveil, in three dimensions, a correlated structural and chemical evolution of Si and SEI. Corroborated with a chemomechanical model, we demonstrate progressive electrolyte permeation and SEI growth along the percolation channel of the nanovoids due to vacancy injection and condensation during the delithiation process. Consequently, the Si–SEI spatial configuration evolves from the classic ‘core–shell’ structure in the first few cycles to a ‘plum-pudding’ structure following extended cycling, featuring the engulfing of Si domains by the SEI, which leads to the disruption of electron conduction pathways and formation of dead Si, contributing to capacity loss. The spatially coupled interactive evolution model of SEI and active materials, in principle, applies to a broad class of high-capacity electrode materials, leading to a critical insight for remedying the fading of high-capacity electrodes.A correlated structural and chemical evolution of silicon and the solid–electrolyte interphase was unveiled in three dimensions by integrating sensitive elemental tomography, an advanced algorithm and cryogenic scanning transmission electron microscopy. The solid–electrolyte interphase (SEI), a layer formed on the electrode surface, is essential for electrochemical reactions in batteries and critically governs the battery stability. Active materials, especially those with extremely high energy density, such as silicon (Si), often inevitably undergo a large volume swing upon ion insertion and extraction, raising a critical question as to how the SEI interactively responds to and evolves with the material and consequently controls the cycling stability of the battery. Here, by integrating sensitive elemental tomography, an advanced algorithm and cryogenic scanning transmission electron microscopy, we unveil, in three dimensions, a correlated structural and chemical evolution of Si and SEI. Corroborated with a chemomechanical model, we demonstrate progressive electrolyte permeation and SEI growth along the percolation channel of the nanovoids due to vacancy injection and condensation during the delithiation process. Consequently, the Si–SEI spatial configuration evolves from the classic ‘core–shell’ structure in the first few cycles to a ‘plum-pudding’ structure following extended cycling, featuring the engulfing of Si domains by the SEI, which leads to the disruption of electron conduction pathways and formation of dead Si, contributing to capacity loss. The spatially coupled interactive evolution model of SEI and active materials, in principle, applies to a broad class of high-capacity electrode materials, leading to a critical insight for remedying the fading of high-capacity electrodes. A correlated structural and chemical evolution of silicon and the solid–electrolyte interphase was unveiled in three dimensions by integrating sensitive elemental tomography, an advanced algorithm and cryogenic scanning transmission electron microscopy. |
| Author | Jiang, Lin Yi, Ran Song, Miao Li, Xiaolin Zhang, Sulin Zhang, Ji-Guang Jia, Haiping Genc, Arda Wang, Chongmin Chen, Tianwu Tessner, Ted Xue, Dingchuan Pullan, Lee Xu, Yaobin Bouchet-Marquis, Cedric Yoo, Jinkyoung He, Yang |
| Author_xml | – sequence: 1 givenname: Yang surname: He fullname: He, Yang organization: Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory, Beijing University of Science and Technology – sequence: 2 givenname: Lin surname: Jiang fullname: Jiang, Lin organization: Materials and Structural Analysis Division, Thermo Fisher Scientific – sequence: 3 givenname: Tianwu orcidid: 0000-0002-3183-1507 surname: Chen fullname: Chen, Tianwu organization: Department of Engineering Science and Mechanics, Pennsylvania State University – sequence: 4 givenname: Yaobin orcidid: 0000-0002-9945-3514 surname: Xu fullname: Xu, Yaobin organization: Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory – sequence: 5 givenname: Haiping surname: Jia fullname: Jia, Haiping organization: Energy and Environmental Directorate, Pacific Northwest National Laboratory – sequence: 6 givenname: Ran surname: Yi fullname: Yi, Ran organization: Energy and Environmental Directorate, Pacific Northwest National Laboratory – sequence: 7 givenname: Dingchuan surname: Xue fullname: Xue, Dingchuan organization: Department of Engineering Science and Mechanics, Pennsylvania State University – sequence: 8 givenname: Miao surname: Song fullname: Song, Miao organization: Physical and Computational Science Directorate, Pacific Northwest National Laboratory – sequence: 9 givenname: Arda surname: Genc fullname: Genc, Arda organization: Materials and Structural Analysis Division, Thermo Fisher Scientific – sequence: 10 givenname: Cedric surname: Bouchet-Marquis fullname: Bouchet-Marquis, Cedric organization: Materials and Structural Analysis Division, Thermo Fisher Scientific – sequence: 11 givenname: Lee surname: Pullan fullname: Pullan, Lee organization: Materials and Structural Analysis Division, Thermo Fisher Scientific – sequence: 12 givenname: Ted surname: Tessner fullname: Tessner, Ted organization: Materials and Structural Analysis Division, Thermo Fisher Scientific – sequence: 13 givenname: Jinkyoung orcidid: 0000-0002-9578-6979 surname: Yoo fullname: Yoo, Jinkyoung email: jyoo@lanl.gov organization: Center for Integrated Nanotechnologies, Los Alamos National Laboratory – sequence: 14 givenname: Xiaolin orcidid: 0000-0002-7728-0157 surname: Li fullname: Li, Xiaolin email: xiaolin.li@pnnl.gov organization: Energy and Environmental Directorate, Pacific Northwest National Laboratory – sequence: 15 givenname: Ji-Guang orcidid: 0000-0001-7343-4609 surname: Zhang fullname: Zhang, Ji-Guang organization: Energy and Environmental Directorate, Pacific Northwest National Laboratory – sequence: 16 givenname: Sulin orcidid: 0000-0003-4429-8235 surname: Zhang fullname: Zhang, Sulin email: suz10@psu.edu organization: Department of Engineering Science and Mechanics, Pennsylvania State University – sequence: 17 givenname: Chongmin orcidid: 0000-0003-3327-0958 surname: Wang fullname: Wang, Chongmin email: chongmin.wang@pnnl.gov organization: Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory |
| BackLink | https://www.ncbi.nlm.nih.gov/pubmed/34326526$$D View this record in MEDLINE/PubMed https://www.osti.gov/servlets/purl/1833249$$D View this record in Osti.gov |
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| Snippet | The solid–electrolyte interphase (SEI), a layer formed on the electrode surface, is essential for electrochemical reactions in batteries and critically governs... The solid-electrolyte interphase (SEI), a layer formed on the electrode surface, is essential for electrochemical reactions in batteries and critically governs... |
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| SubjectTerms | 639/301/299/161/891 639/4077/4079/891 Algorithms batteries Chemical evolution Chemical reactions Chemistry and Materials Science Condensates Control stability Cycles Electrochemistry Electrode materials Electrodes Electrolytes Evolution Fading Flux density Interphase MATERIALS SCIENCE Nanotechnology Nanotechnology and Microengineering Percolation Scanning electron microscopy Scanning transmission electron microscopy Silicon Tomography Transmission electron microscopy |
| Title | Progressive growth of the solid–electrolyte interphase towards the Si anode interior causes capacity fading |
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