Interfaces between a solid electrolyte and electrodes in ASSBs need to be carefully engineered to enable high performance. This study leverages advanced characterization techniques (atomic force microscopy and synchrotron X-ray transmission microscopy) as well as computational tools to understand the mechanical response of electrode|electrolyte interfaces in model hybrid electrolyte systems. The impact of mechanical properties of the extrinsic interfaces on electrochemical performance is evaluated. Active control of interfacial properties is identified as a potential route to engineer high-performance solidstate batteries.
Hybrid solid state electrolyte structure was imaged using synchrotron nanotomography. Accessible surface area of ceramic particles in the electrolytes governs ion transport.
High-rate capable, reversible lithium metal anodes are necessary for next generation energy storage systems. In situ tomography of Li|LLZO|Li cells is carried out to track morphological transformations in Li metal electrodes. Machine learning enables tracking the lithium metal morphology during galvanostatic cycling. Nonuniform lithium electrode kinetics are observed at both electrodes during cycling. Hot spots in lithium metal are correlated with microstructural anisotropy in LLZO. Mesoscale modeling reveals that regions with lower effective properties (transport and mechanical) are nuclei for failure. Advanced visualization combined with electrochemistry represents an important pathway toward resolving non-equilibrium effects that limit rate capabilities of solid-state batteries.
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