Simulation of the Deformation for Cycling Chemo-Mechanically Coupled Battery Active Particles with Mechanical Constraints

TL;DR

This paper develops a coupled chemical-mechanical simulation model for battery particles with mechanical constraints, revealing how boundary limitations affect stress and phase distribution during charge cycles.

Contribution

It introduces a variational inequality boundary condition into a continuum model, enabling simulation of limited particle swelling in lithium-ion batteries.

Findings

Boundary constraints significantly influence maximum stress levels.

The obstacle can induce lithium-poor regions in particles.

Adaptive algorithms improve simulation efficiency.

Abstract

Next-generation lithium-ion batteries with silicon anodes have positive characteristics due to higher energy densities compared to state-of-the-art graphite anodes. However, the large volume expansion of silicon anodes can cause high mechanical stresses, especially if the battery active particle cannot expand freely. In this article, a thermodynamically consistent continuum model for coupling chemical and mechanical effects of electrode particles is extended by a change in the boundary condition for the displacement via a variational inequality. This switch represents a limited enlargement of the particle swelling or shrinking due to lithium intercalation or deintercalation in the host material, respectively. For inequality constraints as boundary condition a smaller time step size is need as well as a locally finer mesh. The combination of a primal-dual active set algorithm, interpreted as semismooth Newton method, and a spatial and temporal adaptive algorithm allows the efficient numerical investigation based on a finite element method. Using the example of silicon, the chemical and mechanical behavior of one- and two-dimensional representative geometries for a charge-discharge cycle is investigated. Furthermore, the efficiency of the adaptive algorithm is demonstrated. It turns out that the size of the gap has a significant influence on the maximal stress value and the slope of the increase. Especially in two dimension, the obstacle can cause an additional region with a lithium-poor phase.