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New battery technologies are currently under development, and among them, all-solid-state batteries should deliver better electrochemical performance and enhanced safety. Composite solid electrolytes, combining a solid polymer electrolyte (SPE) and a ceramic electrolyte (CE), should then provide high ionic conductivity coupled to high mechanical stability. To date, this synergy has not yet been reached due to the complexity of the Li-ion transport within the hybrid solid electrolyte, especially at the SPE/CE interface currently considered the limiting step. Yet, there is no proper kinetic model to elucidate the parameters influencing this interfacial barrier. The limited understanding of the SPE/CE interface can be partly explained by scattered SPE/CE interface resistances reported in the literature as well as the lack of systematic studies. Herein, we propose a systematic study of the effect on the SPE/CE interfacial resistance of chemical and thermal treatments of a model LATP-based ceramic based on a methodology relying on electrochemical impedance spectroscopy (EIS) and X-ray photoemission spectroscopy (XPS). The results provide different levers for the optimization of this interface and valuable insights into experimental precautions needed to obtain more reproducible results.
Mangani et al. (Tue,) studied this question.