Complexions at the Electrolyte/Electrode Interface in Solid Oxide Cells

Rapid deactivation presently limits a wide spread use of high-temperature solid oxide cells (SOCs) as otherwise highly efficient chemical energy converters. With deactivation triggered by the ongoing conversion reactions, an atomic-scale understanding of the active triple-phase boundary (TPB) between electrolyte, electrode and gas phase is essential to increase cell performance. Here we use a multi-method approach comprising transmission electron microscopy and first-principles calculations and molecular simulations to untangle the atomic arrangement of the prototypical SOC interface between a lanthanum strontium manganite (LSM) anode and an yttria-stabilized zirconia (YSZ) electrolyte. We identify an interlayer of self-limited width with partial amorphization and strong compositional gradient, thus exhibiting the characteristics of a complexion that is stabilized by the confinement between two bulk phases. This offers a new perspective to understand the function of SOCs at the atomic scale. Moreover, it opens up a hitherto unrealized design space to tune the conversion efficiency.