Unveiling Surface Chemistry of Ultrafast-Sintered LLZO Solid-State Electrolytes for High-Performance Li-Garnet Solid-State Batteries

Unveiling Surface Chemistry of Ultrafast-Sintered LLZO Solid-State Electrolytes for High-Performance Li-Garnet Solid-State Batteries

© 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), 22 vom: 26. Nov., Seite 11254-11263
1. Verfasser: Zhang, Huanyu (VerfasserIn)
Weitere Verfasser: Klimpel, Matthias, Wieczerzak, Krzysztof, Dubey, Romain, Okur, Faruk, Michler, Johann, Jeurgens, Lars P H, Chernyshov, Dmitry, van Beek, Wouter, Kravchyk, Kostiantyn V, Kovalenko, Maksym V
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.
Ultrafast (UF) sintering emerges as a game-changing sintering methodology for fabricating Li7La3Zr2O12 (LLZO) solid-state electrolytes, representing a pivotal stride toward the advancement and prospective commercialization of Li-garnet solid-state batteries. Despite its widespread use in the fabrication of LLZO ceramics, the chemical composition of the UF-sintered LLZO surface remains largely unexplored. This study presents an in-depth analysis of the surface chemistry of UF-sintered LLZO using comprehensive techniques, including depth-profiling X-ray photoelectron spectroscopy (XPS) and focused-ion-beam time-of-flight secondary ion mass spectroscopy (FIB-TOF-SIMS). Our investigation uncovers a striking difference between the surface of UF-sintered and conventionally sintered LLZO, revealing predominant surface contamination by Li2O up to ca. 40 nm depth in the case of UF processing. Comparative synchrotron X-ray diffraction data during UF and conventional sintering elucidate the origin of surface contamination. We propose a viable solution to this issue through an additional heat treatment (HT) step at 900 °C after UF sintering, as corroborated by XPS and FIB-TOF-SIMS measurements. Furthermore, we present a comparative assessment of the electrochemical performance of Li/LLZO/Li symmetric cells based on UF-sintered LLZO pellets, both with and without the post-HT step, underscoring the pivotal role of an uncontaminated LLZO surface
Beschreibung:Date Revised 02.12.2024
published: Electronic-eCollection
Citation Status PubMed-not-MEDLINE
ISSN:0897-4756
DOI:10.1021/acs.chemmater.4c02351