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Normal operations of electrochemical devices such as solid oxide fuel cells(SOFC), solid oxide electrolyzer cells (SOEC) and lithium ion batteries (LIB)sometimes fail because of unexpected formation of internal phases. These phasesinclude oxygen bubbles at grain boundaries inside the zirconia electrolyte ofSOEC, isolated Li metal islands inside the (garnet type) Li7La3Zr2O12electrolyte of all-solid-state LIB, and similar Na metal islands inside theNa-beta-alumina and NASICON electrolytes of Na-S batteries. Remarkably,although the devices can operate in both polarities, the propensity for failuredepends on the polarity. Here we explain these and other phenomena in nominallyionic solid electrolytes and mixed-conducting electrodes in simplethermodynamic and kinetic terms: the unexpected internal phases are caused by alarge potential jump that is needed to push a constant ion or electron flowthrough its internal transport bottleneck. Definite rules for internal phaseformation including its polarity dependence are formulated to help predict andmitigate it, which leads to microstructural instability, efficiencydeterioration and breakdown.

Potential jumps at transport bottlenecks cause instability of nominally ionic solid electrolytes in electrochemical cells