In this talk, we report on a series of hybrid electrolytes made from a high concentration (HC) electrolyte. These electrolytes are evaluated by using vibrational spectroscopy and electrochemical and force measurements. We show the presence of a surface-confinement effect in the HC electrolytes and the presence of layers, the structure of which changes with applied potential.. Vibrational spectroscopy shows that the composition of the double layer also changes with potential, where the anion is enriched at positive and cationic species enriched at negative potentials, respectively. The presence of divalent or diluent molecules changes the layering effect. HC electrolytes are utilized in both symmetric and full cells with different cathode chemistries. HC electrolytes used with Li2S cathodes is beneficial for achieving high active material utilization, maintaining intimate interfacial contact, and providing buffer space for volume contraction and expansion. The HC-enabled Li2S cell exhibited superior cycling performance compared to all-solid-state cells in terms of loading, Li2S utilization, and cycling stability. Finally, we discuss the use of hybrid electrolytes to enable other cathode chemistries, such as those involving organics molecules like lithium rhodizonate (Li2C6O6) , a cathode chemistry which shows improved reversibility under conditions of high applied mechanical loads.

High concentration electrolytes for lithium and Mulitvalent batteries

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ACS Fall 2022

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