Unveiling Surface Chemistry of Ultrafast-Sintered LLZO Solid-State Electrolytes for High-Performance Li-Garnet Solid-State Batteries
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2024-11-26
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Journal Article
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Abstract
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 degrees 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.
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published
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36 (22)
Pages / Article No.
11254 - 11263
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American Chemical Society
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03934 - Kovalenko, Maksym / Kovalenko, Maksym