journal article·2025-03Open access

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

Walter Cistjakov, Johanna Hoppe, Jinkwan Jung, Fridolin Röder, Hee‐Tak Kim, Ulrike Krewer

Advanced Materials Interfaces· Volume 12· Issue 5

Abstract

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.
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Research context

OpenAlex topics: Advanced Battery Materials and Technologies · Advancements in Battery Materials · Advanced Battery Technologies Research

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Institute of Energy and Process Systems Engineering Technische Universität Braunschweig Langer Kamp 19b Braunschweig 38106 Lower Saxony Germany

Cluster of Excellence “SE2A – Sustainable and Energy‐Efficient Aviation” Technische Universität Braunschweig Hermann‐Blenk‐Str. 42 Braunschweig 38108 Lower Saxony Germany

Transformation Pathways Potsdam Institute for Climate Impact Research (PIK) Telegrafenberg A 3 Potsdam 14412 Brandenburg Germany

Department of Chemical and Biomolecular Engineering Korean Advanced Institute of Science and Technology 291 Daehak‐ro Daejeon 34141 South Korea

Bavarian Center for Battery Technology (BayBatt) University of Bayreuth Weiherstraße 26 Bayreuth 95448 Bavaria Germany

Institute for Applied Materials – Electrochemical Technologies Karlsruhe Institute of Technology Adenauerring 20b Karlsruhe 76131 Baden‐Wuerttemberg Germany

Funding

Deutsche Forschungsgemeinschaft

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