Trapping and imaging dynamic battery nanointerfaces via electrified cryo-EM.

Abstract

The electrified interface between a liquid and a solid underpins diverse phenomena, from ion-transfer during battery operation to action potentials enabling biological communication. However, conventional tools are blind to the nanoscale dynamics of this metastable interface. Here, we leverage electrified cryo-electron microscopy (eCryo-EM), a technique that rapidly freezes and kinetically traps these dynamic, nonequilibrium states during battery operation for nanoscale characterization. Collective snapshots of the electrified interface at controlled time intervals quantifies early-stage growth kinetics of the solid electrolyte interphase (SEI), a passivation film that governs electron and ion transport. Unexpectedly, the diffusivity of charged species of the two SEI films with differing chemistry and performance are estimated to be within 10% of the other, indicated by the slope of their diffusion-limited SEI growth regimes. Instead, the slope of the reaction-limited SEI growth regimes differs by a factor of 3, suggesting that lowered reactivity of the high-performance electrolyte is largely responsible for its high coulombic efficiency.