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

Title data

Gerasimov, Michail ; Soto, Fernando A. ; Wagner, Janika ; Baakes, Florian ; Guo, Ningxuan ; Ospina-Acevedo, Francisco ; Röder, Fridolin ; Balbuena, Perla B. ; Krewer, Ulrike:
Species Distribution During Solid Electrolyte Interphase Formation on Lithium Using MD/DFT-Parameterized Kinetic Monte Carlo Simulations.
In: The Journal of Physical Chemistry C. Vol. 127 (2023) Issue 10 . - pp. 4872-4886.
ISSN 1932-7455

Abstract in another language

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. At the lithium surface, an inorganic layer of lithium fluoride and then lithium carbonate is observed, followed by an organic, more porous SEI layer consisting of lithium ethylene dicarbonate. Simulations further reveal the strong prevalence of corrosion processes of the metal, which provide more than 99% of the lithium for the SEI reaction processes. The salt contributes less than 1% to the SEI formation. Additionally, SEI formation below and above the initial interface was observable. The here presented novel modeling approach allows an unprecedented in-depth analysis of processes during native SEI formation that can be used to improve design for high battery performance and durability.

Further data

Item Type: Article in a journal
Refereed: Yes
Institutions of the University: Faculties > Faculty of Engineering Science > Junior Professor Methods of Managing Batteries > Junior Professor Methods of Managing Batteries - Juniorprof. Dr.-Ing. Fridolin Röder
Research Institutions > Central research institutes > Bayerisches Zentrum für Batterietechnik - BayBatt
Result of work at the UBT: Yes
DDC Subjects: 600 Technology, medicine, applied sciences > 620 Engineering
Date Deposited: 15 Mar 2024 07:14
Last Modified: 15 Mar 2024 07:14