Lithium electrode growth regime due to solid electrolyte interphase: A multiphase-field approach

The solid electrolyte interphase (SEI) plays a critical role in controlling the current distribution at the lithium electrode/electrolyte interface. The heterogeneous nature of lithium deposition leads to dendrite formation. To address this, we develop a multiphase-field model to investigate the role of a heterogeneous SEI in dendrite nucleation during electrodeposition. We first propose a qualitative study to characterize lithium growth regimes and define an observable mechanism to identify SEI failure modes leading to dendrite nucleation. Finally, a parametric study of the SEI structure highlights the key characteristics that can drive the nucleation of lithium dendrite. • A multiphase field model describes chemical complexity at lithium metal interfaces. • The model reveals mechanisms driving lithium dendrite nucleation. • Two distinct dendrite nucleation modes are identified and characterized. • Key parameters controlling dendrite nucleation are quantified.