Transport of secondary carriers in a solid lithium-ion conductor

Inorganic-solid lithium electrolytes are typically thought of as single-ion conductors, but the presence secondary carriers can strongly affect their performance. Conventional descriptions multi-carrier transport neglect both interactions between mobile species and stress diffusion — phenomena which markedly impact electrical response. We apply irreversible thermodynamics to develop a chemomechanical model for elastic-solid ionic conductors containing two ions. simulate lithium-ion conducting Li5La3Nb2O12 (LLNO) garnet oxide, material within experiments have shown that protons be freely substituted form Li5(1−y)H5yLa3Nb2O12. When subjected current, we find proton-substituted LLNO exhibits bulk polarization, whose extent is partially controlled by cation/cation interactions. Secondary segregate naturally if global concentration low, accumulating in thin boundary layer near cathode. quantify limiting current Sand’s time, analyze experimental data show how competitive proton affects