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

Janika Wagner-Henke, Dacheng Kuai, Michail Gerasimov, Fridolin Röder, Perla B. Balbuena and Ulrike Krewer ()
Additional contact information
Janika Wagner-Henke: Karlsruhe Institute of Technology
Dacheng Kuai: Texas A&M University
Michail Gerasimov: Karlsruhe Institute of Technology
Fridolin Röder: University of Bayreuth
Perla B. Balbuena: Texas A&M University
Ulrike Krewer: Karlsruhe Institute of Technology

Nature Communications, 2023, vol. 14, issue 1, 1-16

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 Li2CO3 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.

Date: 2023
References: View complete reference list from CitEc
Citations:

Downloads: (external link)
https://www.nature.com/articles/s41467-023-42212-7 Abstract (text/html)

Related works:
This item may be available elsewhere in EconPapers: Search for items with the same title.

Export reference: BibTeX RIS (EndNote, ProCite, RefMan) HTML/Text

Persistent link: https://EconPapers.repec.org/RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-42212-7

Ordering information: This journal article can be ordered from
https://www.nature.com/ncomms/

DOI: 10.1038/s41467-023-42212-7

Access Statistics for this article

Nature Communications is currently edited by Nathalie Le Bot, Enda Bergin and Fiona Gillespie

More articles in Nature Communications from Nature
Bibliographic data for series maintained by Sonal Shukla () and Springer Nature Abstracting and Indexing ().