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Insight into the Impact of Electrolyte on Passivation of Lithium–Sulfur Cathodes

Cistjakov, Walter 1; Hoppe, Johanna; Jung, Jinkwan; Röder, Fridolin; Kim, Hee-Tak; Krewer, Ulrike ORCID iD icon 1
1 Institut für Angewandte Materialien – Elektrochemische Technologien (IAM-ET1), Karlsruher Institut für Technologie (KIT)

Abstract:

One of the remaining challenges for lithium–sulfur batteries toward practical application is early cathode passivation by the insulating discharge product: Li2S. To understand how to best mitigate passivation and minimize related performance loss, a kinetic Monte–Carlo model for Li2S crystal growth from solution is developed. The key mechanisms behind the strongly different natures of Li2S layer growth, structure, and morphology for salts with different (DN) are revealed. LiTFSI electrolyte in dimethyl ether leads to lateral Li2S growth on carbon and fast passivation because it increases the Li2S precipitation-to-dissolution probability on carbon relative to Li2S. In contrast, LiBr electrolyte has a higher DN and yields a particle-like structure due to a significantly higher precipitation-to-dissolution probability on Li2S compared to carbon. The resulting large number of Li2S sites further favors particle growth, leading to low passivation. This study is able to identify the key parameters of the electrolyte and substrate material to tune Li2S morphology and growth to pave the way for optimized performance.

Zugehörige Institution(en) am KIT Institut für Angewandte Materialien – Elektrochemische Technologien (IAM-ET1)
Publikationstyp Zeitschriftenaufsatz
Publikationsmonat/-jahr 03.2025
Sprache Englisch
Identifikator ISSN: 2196-7350
KITopen-ID: 1000175862
Erschienen in Advanced Materials Interfaces
Verlag John Wiley and Sons
Band 12
Heft 5
Seiten Art.-Nr.: 2400632
Vorab online veröffentlicht am 14.10.2024
Nachgewiesen in OpenAlex
Web of Science
Scopus
Dimensions
Relationen in KITopen
Globale Ziele für nachhaltige Entwicklung Ziel 7 – Bezahlbare und saubere Energie

Verlagsausgabe §
DOI: 10.5445/IR/1000175862
Veröffentlicht am 04.11.2024
Seitenaufrufe: 35
seit 04.11.2024
Downloads: 18
seit 14.11.2024
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