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Species Distribution During Solid Electrolyte Interphase Formation on Lithium Using MD/DFT-Parameterized Kinetic Monte Carlo Simulations

Gerasimov, Michail ORCID iD icon 1; Soto, Fernando A.; Wagner, Janika 2; Baakes, Florian ORCID iD icon 2; Guo, Ningxuan; Ospina-Acevedo, Francisco; Röder, Fridolin; Balbuena, Perla B. ; Krewer, Ulrike ORCID iD icon 1
1 Institut für Angewandte Materialien – Elektrochemische Technologien (IAM-ET1), Karlsruher Institut für Technologie (KIT)
2 Karlsruher Institut für Technologie (KIT)

Abstract:

Lithium metal batteries are one of the promising technologies for future energy storage. One open challenge is the generation of a stable and well performing Solid Electrolyte Interphase (SEI) between lithium metal and electrolyte. Understanding the complex interaction of reactions at the lithium surface and the resulting SEI is crucial for knowledge-driven improvement of the SEI. This study reveals the internal species distribution and geometrical aspects of the native SEI during formation by model-based analysis. To achieve this, a combination of molecular dynamics, density functional theory, and stand-alone 3D-kinetic Monte Carlo simulations is used. The kinetic Monte Carlo model determines the SEI growth features over a long time and length scale so that the SEI can be analyzed quantitatively. The simulation confirms the frequently postulated layered SEI structure arising from the decomposition of an ethylene carbonate/lithium hexafluorophosphate (2 M) electrolyte with lithium metal. These layers are not clearly separated, which is contrary to what is often reported. The gradient distribution of the species within the SEI therefore corresponds to a partly mosaic structured SEI at the borders of the layers. ... mehr


Verlagsausgabe §
DOI: 10.5445/IR/1000157185
Veröffentlicht am 11.04.2023
Originalveröffentlichung
DOI: 10.1021/acs.jpcc.2c05898
Scopus
Zitationen: 18
Web of Science
Zitationen: 12
Dimensions
Zitationen: 16
Cover der Publikation
Zugehörige Institution(en) am KIT Institut für Angewandte Materialien – Elektrochemische Technologien (IAM-ET1)
Publikationstyp Zeitschriftenaufsatz
Publikationsdatum 16.03.2023
Sprache Englisch
Identifikator ISSN: 1932-7447, 1932-7455
KITopen-ID: 1000157185
Erschienen in The Journal of Physical Chemistry C
Verlag American Chemical Society (ACS)
Band 127
Heft 10
Seiten 4872–4886
Vorab online veröffentlicht am 01.03.2023
Nachgewiesen in Scopus
Dimensions
Web of Science
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