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Model Studies on the Formation of the Solid Electrolyte Interphase: Reaction of Li with Ultrathin Adsorbed Ionic-Liquid Films and Co$_{3}$O$_{4}$(111) Thin Films

Forster-Tonigold, Katrin; Kim, Jihyun; Bansmann, Joachim; Groß, Axel; Buchner, Florian

Abstract:
In this work we aim towards the molecular understanding of the solid electrolyte interphase (SEI) formation at the electrode electrolyte interface (EEI). Herein, we investigated the interaction between the battery‐relevant ionic liquid (IL) 1‐butyl‐1‐methylpyrrolidinium bis(trifluoromethylsulfonyl)imide (BMP‐TFSI), Li and a Co$_{3}$O$_{4}$(111) thin film model anode grown on Ir(100) as a model study of the SEI formation in Li‐ion batteries (LIBs). We employed mostly X‐ray photoelectron spectroscopy (XPS) in combination with dispersion‐corrected density functional theory calculations (DFT‐D3). If the surface is pre‐covered by BMP‐TFSI species (model electrolyte), post‐deposition of Li (Li$^{+}$ ion shuttle) reveals thermodynamically favorable TFSI decomposition products such as LiCN, Li$_{2}$NSO$_{2}$CF$_{3}$, LiF, Li$_{2}$S, Li$_{2}$O$_{2}$, Li$_{2}$O, but also kinetic products like Li$_{2}$NCH$_{3}$C$_{4}$H$_{9}$ or LiNCH$_{3}$C$_{4}$H$_{9}$ of BMP. Simultaneously, Li adsorption and/or lithiation of Co$_{3}$O$_{4}$(111) to LinCo$_{3}$O$_{4}$ takes place due to insertion via step edges or defects; a partial transformation to CoO cannot be excluded. ... mehr

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Verlagsausgabe §
DOI: 10.5445/IR/1000130348
Veröffentlicht am 10.03.2021
Cover der Publikation
Zugehörige Institution(en) am KIT Helmholtz-Institut Ulm (HIU)
Publikationstyp Zeitschriftenaufsatz
Publikationsdatum 03.03.2020
Sprache Englisch
Identifikator ISSN: 1439-4235, 1439-7641
KITopen-ID: 1000130348
Erschienen in ChemPhysChem
Verlag Wiley
Band 22
Heft 5
Seiten 441-454
Schlagwörter cobalt oxide; density functional theory; ionic liquids; solid electrolyte interphase; surface chemistry
Nachgewiesen in Web of Science
Scopus
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