Publication date: 10th April 2024
All Solid-State Batteries (ASSBs) are looked as the most promising technology to go beyond the limitation of LiBs. The presence of a solid electrolyte may reduce the propagation of dendrites, and absence of a flammable liquid eases the explosion risk in case of thermal runaway. This kind of batteries, denominated Gen4b, couples the solid electrolyte with Li metal (theoretical specific capacity: 3860 mA h/g) and high voltage cathodes, which use, allowed by the low flammable risk, will in addition increase the gravimetric and volumetric energy density beyond incumbent LIBs[1].
Sulfide-based materials emerge from the historical proposed ceramic materials, such oxides, as a favorable candidate to be used as solid electrolyte in ASSBs in view of their promising performance and ease of manufacturing. Sulfides are characterized by high ionic conductivity (above 1mS/cm at RT), they show mechanical strength together with easy processability, which allows their manufacturing from densification under pressure at room temperature (an advantage towards oxides, which require high sintering temperature). However, their difficulty to withstand high current density and long-term cycling, as well as their sensitivity to moisture are hampering their entrance into the battery market.
This work aims to provide a better understanding of the transport properties of sulfide-based ASSBs, for which, as a case of study, argyrodite Li6PS5Cl separators are considered. First the conduction properties were analyzed and correlated with Li-ion mobility in the electrolyte itself. Secondly the interfacial processes taking place at the battery level were investigated, for this purpose, distribution of relaxation times has been applied[2,3]. This technique allows to correlate the factors determining the cell performance to the various impedance sources happening at the Li|electrolyte and cathode|electrolyte interfaces. As result, the degradation process at the electrolyte interfaces have been followed during cycling, giving precious insight on the parasitic reaction happening during real operating condition.
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