Publication date: 10th April 2024
The use of inorganic ceramic solid electrolytes (SEs) to produce all-solid-state lithium batteries (ASSLBs) can overcome the safety issues related to conventional liquid electrolytes and enable Li batteries to operate at higher voltage. To make this happen, one of the most crucial requirements for the SE is to possess a large electrochemical stability window (ESW). Li7La3Zr2O12 (LLZO) solid electrolyte has attracted a lot of attention given its high ionic conductivity and because it was first reported with a very wide ESW (0–9 V vs. Li+/Li). It was not until recently that this value of the ESW was challenged, mainly proving that the oxidation of LLZO happened at a much earlier potential than 9 V. In the same line of thought, our work describes a methodology to accurately determine the ESW of doped M:LLZO (M = Al, Ta and Nb). The ESW of M:LLZO was found to be identical for all three dopants and much narrower than previously documented, on both reduction and oxidation sides. The reduction reaction was evidenced through ex situ 7Li nuclear magnetic resonance and operando powder X-ray diffraction analyses.
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