Effects of reversible chemical reaction on Li diffusion and stresses in spherical composition-gradient electrodes

Abstract

Composition-gradient electrode materials have been proven to be one of the most promising materials in lithium-ion battery. To study the mechanism of mechanical degradation in spherical composition-gradient electrodes, the finite deformation theory and reversible chemical theory are adopted. In homogeneous electrodes, reversible electrochemical reaction may increase the magnitudes of stresses. However, reversible electrochemical reaction has different influences on stresses in composition-gradient electrodes, resulting from three main inhomogeneous factors - forward reaction rate, backward reaction rate, and reaction partial molar volume. The decreasing transition form of forward reaction rate, increasing transition form of backward reaction rate, and increasing transition form of reaction partial molar volume can reduce the magnitudes of stresses. As a result, capacity fading and mechanical degradation are reduced by taking advantage of the effects of inhomogeneous factors.