Large Plastic Deformation in High‐Capacity Lithium‐Ion Batteries Caused by Charge and Discharge

Abstract

Evidence has accumulated recently that a high‐capacity electrode of a lithium‐ion battery may not recover its initial shape after a cycle of charge and discharge. Such a plastic behavior is studied here by formulating a theory that couples large amounts of lithiation and deformation. The homogeneous lithiation and deformation in a small element of an electrode under stresses is analyzed within nonequilibrium thermodynamics, permitting a discussion of equilibrium with respect to some processes, but not others. The element is assumed to undergo plastic deformation when the stresses reach a yield condition. The theory is combined with a diffusion equation to analyze a spherical particle of an electrode being charged and discharged at a constant rate. When the charging rate is low, the distribution of lithium in the particle is nearly homogeneous, the stress in the particle is low, and no plastic deformation occurs. When the charging rate is high, the distribution of lithium in the particle is inhomogeneous, and the stress in the particle is high, possibly leading to fracture and cavitation.