Publications

Spatially Resolved Potential and Li-Ion Distributions Reveal Performance-Limiting Regions in Solid-State Batteries

Fuller, Elliot J.; Strelcov, Evgheni; Weaver, Jamie L.; Swift, Michael W.; Sugar, Joshua D.; Kolmakov, Andrei; Zhitenev, Nikolai; McClelland, Jabez J.; Qi, Yue; Dura, Joseph A.; Talin, A.A.

The performance of solid-state electrochemical systems is intimately tied to the potential and lithium distributions across electrolyte-electrode junctions that give rise to interface impedance. Here, we combine two operando methods, Kelvin probe force microscopy (KPFM) and neutron depth profiling (NDP), to identify the rate-limiting interface in operating Si-LiPON-LiCoO2 solid-state batteries by mapping the contact potential difference (CPD) and the corresponding Li distributions. The contributions from ions, electrons, and interfaces are deconvolved by correlating the CPD profiles with Li-concentration profiles and by comparisons with first-principles-informed modeling. We find that the largest potential drop and variation in the Li concentration occur at the anode-electrolyte interface, with a smaller drop at the cathode-electrolyte interface and a shallow gradient within the bulk electrolyte. Correlating these results with electrochemical impedance spectroscopy following battery cycling at low and high rates confirms a long-standing conjecture linking large potential drops with a rate-limiting interfacial process.