Publication date: 10th April 2024
A large proportion of the batteries marketed worldwide are Li-ion batteries, which generally use a mixture of lithium salts and organic liquid as an electrolyte (LE). But this technology poses several issues, the main one being safety due to the high flammability of the organic solvent, and the energy density also reaches limits with LE since Li metal cannot be used as negative electrode. All solid-state batteries could provide a suitable alternative by replacing LE with a solid electrolyte that is less flammable and allows lithium metal to be used as a negative electrode to increase energy density [1]. The thiophosphate materials family is one of the most promising ones owing to their good ionic and suitable mechanical properties. However, the numerous solid-solid interfaces especially the electrode/electrolyte ones are complex to handle as it is one of the principal causes of electrochemical fading [2]. Especially on the positive electrode, the optimal contact between the two solids promotes the chemical decomposition due to the contact between an oxide (electronic conductor) and a thiophosphate (ionic conductor), leading to the creation of several insulating products that generate an increase in impedance. Composite electrode engineering is not an easy task due to the intrinsic engineering of the solid-state batteries where there must be no (or almost no) porosity after sintering to improve wetting between the active material and the electrolyte. Indeed, the contact is the sole option to guarantee an optimized electrochemical activities and transport properties [3]. Here, we proposed to investigate an Li6PS5Cl/NCM523 composite electrode prior cycling to understand the impact of the electrode engineering such as the ratio of the solid electrolyte/electroactive materials, the nature of the electronic/ionic conductor. The investigation will be carried out by means of electrochemical impedance spectroscopy performed at different temperature coupled with several advanced characterizations performed at ESRF synchrotron (XRD, XAS). The goal being to find the optimal ratio to ensure a proper ionic and electronic conductivities while giving satisfactory electrochemical performance.
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