Controlling the roughening of growing electrochemical interfaces using temperature gradients.

Abstract

The excessive dendritic development during the electrochemical evolution of the microstructures in rechargeable batteries can ultimately cause a short circuit, thermal instability, or runaway, and loss of active material. We initially develop a computational framework to quantify the bias of the electrodeposition on the roughened interface favoring the convex zones. Subsequently, we impose a countering temperature effect to enhance the diffusion on the trailing concave zones. Consequently, we establish a stability criterion for controlling surface roughening where the visualized space of parameters establishes a relationship between the geometry of the interface, the physical properties of the electrolyte, and the charging conditions. The developed framework could be useful for controlling the propagation of the microstructures and the prevention of runaway, during prolonged cycles, particularly when the surface roughness gets pronounced in the later stage of cycle life.