Insights into the LiMn2O4 Cathode Stability in Aqueous Electrolytes

© 2024 The Authors. Published by American Chemical Society.

Bibliographische Detailangaben
Veröffentlicht in:Chemistry of materials : a publication of the American Chemical Society. - 1998. - 36(2024), 12 vom: 25. Juni, Seite 6144-6153
1. Verfasser: Gonzalez-Rosillo, Juan Carlos (VerfasserIn)
Weitere Verfasser: Guc, Maxim, Liedke, Maciej Oskar, Butterling, Maik, Attallah, Ahmed G, Hirschmann, Eric, Wagner, Andreas, Izquierdo-Roca, Victor, Baiutti, Federico, Morata, Alex, Tarancón, Albert
Format: Online-Aufsatz
Sprache:English
Veröffentlicht: 2024
Zugriff auf das übergeordnete Werk:Chemistry of materials : a publication of the American Chemical Society
Schlagworte:Journal Article
Beschreibung
Zusammenfassung:© 2024 The Authors. Published by American Chemical Society.
LiMn2O4 (LMO) cathodes present large stability when cycled in aqueous electrolytes, contrasting with their behavior in conventional organic electrolytes in lithium-ion batteries (LIBs). To elucidate the mechanisms underlying this distinctive behavior, we employ unconventional characterization techniques, including variable energy positron annihilation lifetime spectroscopy (VEPALS), tip-enhanced Raman spectroscopy (TERS), and macro-Raman spectroscopy (with tens of μm-size laser spot). These still rather unexplored techniques in the battery field provide complementary information across different length scales, revealing previously hidden features. VEPALS offers atomic-scale insights, uncovering cationic defects and subnanometer pores that tend to collapse with cycling. TERS, operating in the nanometric range at the surface, captured the presence of Mn3O4 and its dissolution with cycling, elucidating dynamic changes during operation. Additionally, TERS highlights the accumulation of SO4 2- at grain boundaries. Macro-Raman spectroscopy focuses on the micrometer scale, depicting small changes in the cathode's long-range order, suggesting a slow but progressive loss of crystalline quality under operation. Integrating these techniques provides a comprehensive assessment of LMO cathode stability in aqueous electrolytes, offering multifaceted insights into phase and defect evolution that can help to rationalize the origin of such stability when compared with conventional organic electrolytes. Our findings advance the understanding of LMO behavior in aqueous environments and provide guidelines for its development for next-generation LIBs
Beschreibung:Date Revised 02.07.2024
published: Electronic-eCollection
Citation Status PubMed-not-MEDLINE
ISSN:0897-4756
DOI:10.1021/acs.chemmater.4c00888