Despite the potential advantages promised by solid-state batteries, the success of solid-state electrolytes has not yet been fully realised. This is due in part to the lower ionic conductivity of solid electrolytes. In many solid superionic conductors, grain boundaries are found to be ionically resistive and hence contribute to this lower ionic conductivity. Additionally, in spite of the hope that solid electrolytes would inhibit lithium filaments, in most scenarios their growth is still observed, and in some polycrystalline systems this is suggested to occur along grain boundaries. It is apparent that grain boundaries affect the performance of solid-state electrolytes, however a deeper understanding is lacking. In this perspective, the current theories relating to grain boundaries in solid-state electrolytes are explored, as well as addressing some of the challenges which arise when trying to investigate their role. Glasses are presented as a possible solution to reduce the effect of grain boundaries in electrolytes. Future research directions are suggested which will aid in both understanding the role of grain boundaries, and diminishing their contribution in cases where they are detrimental.
Lithium alloys have the potential to overcome anode-side challenges in solid state batteries. In this work we synthesize and characterize lithium-rich magnesium alloys, quantifying the changes in mechanical properties, transport, and surface chemistry that impact electrochemical performance. Increases in hardness, stiffness,adhesion, and creep are quantified by nanoindentation as a function of magnesium content. A decrease in diffusivity is quantified with chronopotentiometry and6Li PFG-NMR, and an increase in interfacial impedance due to the presence of magnesium is identified with electrochemical impedance spectroscopy which is correlated with XPS data. Throughout, changes in properties are linked to electrochemical performance. This work provides a framework to investigate other lithium alloy systems.
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