Knowledge-driven design of solid-electrolyte interphases on lithium metal via multiscale modelling

Wagner-Henke, Janika; Kuai, Dacheng; Gerasimov, Michail; Röder, Fridolin; Balbuena, Perla B.; Krewer, Ulrike

doi:10.1038/s41467-023-42212-7

Title: Knowledge-driven design of solid-electrolyte interphases on lithium metal via multiscale modelling

Abstract

Abstract Due to its high energy density, lithium metal is a promising electrode for future energy storage. However, its practical capacity, cyclability and safety heavily depend on controlling its reactivity in contact with liquid electrolytes, which leads to the formation of a solid electrolyte interphase (SEI). In particular, there is a lack of fundamental mechanistic understanding of how the electrolyte composition impacts the SEI formation and its governing processes. Here, we present an in-depth model-based analysis of the initial SEI formation on lithium metal in a carbonate-based electrolyte. Thereby we reach for significantly larger length and time scales than comparable molecular dynamic studies. Our multiscale kinetic Monte Carlo/continuum model shows a layered, mostly inorganic SEI consisting of LiF on top of Li ₂ CO ₃ and Li after 1 µs. Its formation is traced back to a complex interplay of various electrolyte and salt decomposition processes. We further reveal that low local Li ⁺ concentrations result in a more mosaic-like, partly organic SEI and that a faster passivation of the lithium metal surface can be achieved by increasing the salt concentration. Based on this we suggest design strategies for SEI on lithium metal and make an important step towards knowledge-drivenmore » SEI engineering.« less

Authors:

; Kuai, Dacheng;

;

Publication Date:: Thu Oct 26 00:00:00 EDT 2023

Sponsoring Org.:: USDOE

OSTI Identifier:: 2203778

Grant/Contract Number:: AC02-05CH11357

Resource Type:: Published Article

Journal Name:: Nature Communications

Additional Journal Information:: Journal Name: Nature Communications Journal Volume: 14 Journal Issue: 1; Journal ID: ISSN 2041-1723

Publisher:: Nature Publishing Group

Country of Publication:: United Kingdom

Language:: English

Citation Formats


                    Wagner-Henke, Janika, Kuai, Dacheng, Gerasimov, Michail, Röder, Fridolin, Balbuena, Perla B., and Krewer, Ulrike. Knowledge-driven design of solid-electrolyte interphases on lithium metal via multiscale modelling.  United Kingdom: N. p., 2023. 
Web.  doi:10.1038/s41467-023-42212-7.

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                    Wagner-Henke, Janika, Kuai, Dacheng, Gerasimov, Michail, Röder, Fridolin, Balbuena, Perla B., & Krewer, Ulrike. Knowledge-driven design of solid-electrolyte interphases on lithium metal via multiscale modelling.  United Kingdom.  https://doi.org/10.1038/s41467-023-42212-7

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                    Wagner-Henke, Janika, Kuai, Dacheng, Gerasimov, Michail, Röder, Fridolin, Balbuena, Perla B., and Krewer, Ulrike. Thu .  
"Knowledge-driven design of solid-electrolyte interphases on lithium metal via multiscale modelling".  United Kingdom.  https://doi.org/10.1038/s41467-023-42212-7.

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@article{osti_2203778,

  title        = {Knowledge-driven design of solid-electrolyte interphases on lithium metal via multiscale modelling},

  author       = {Wagner-Henke, Janika and Kuai, Dacheng and Gerasimov, Michail and Röder, Fridolin and Balbuena, Perla B. and Krewer, Ulrike},

  abstractNote = {Abstract Due to its high energy density, lithium metal is a promising electrode for future energy storage. However, its practical capacity, cyclability and safety heavily depend on controlling its reactivity in contact with liquid electrolytes, which leads to the formation of a solid electrolyte interphase (SEI). In particular, there is a lack of fundamental mechanistic understanding of how the electrolyte composition impacts the SEI formation and its governing processes. Here, we present an in-depth model-based analysis of the initial SEI formation on lithium metal in a carbonate-based electrolyte. Thereby we reach for significantly larger length and time scales than comparable molecular dynamic studies. Our multiscale kinetic Monte Carlo/continuum model shows a layered, mostly inorganic SEI consisting of LiF on top of Li 2 CO 3 and Li after 1 µs. Its formation is traced back to a complex interplay of various electrolyte and salt decomposition processes. We further reveal that low local Li + concentrations result in a more mosaic-like, partly organic SEI and that a faster passivation of the lithium metal surface can be achieved by increasing the salt concentration. Based on this we suggest design strategies for SEI on lithium metal and make an important step towards knowledge-driven SEI engineering.},

  doi          = {10.1038/s41467-023-42212-7},

  journal      = {Nature Communications},

  number       = 1,

  volume       = 14,

  place        = {United Kingdom},

  year         = {Thu Oct 26 00:00:00 EDT 2023},

  month        = {Thu Oct 26 00:00:00 EDT 2023}

}

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