Phase-field modeling and computational design of structurally stable NMC materials

Lithium Nickel Manganese Cobalt Oxides (NMC) are one of the most used cathode materials in lithium-ion batteries, and they will become more relevant in the following years due to their potential in electric vehicles. Unfortunately, this material experiences microcracking during the battery operation due to the volume variations, which is detrimental to the battery performance and limits the lifetime of the electrodes. Thus, understanding mechanical degradation is fundamental for the development of advanced batteries with improved capacity and limited degradation. In this work, we propose a chemo-mechanical model, including a stochastic phase-field fracture approach, to design structurally stable NMC electrodes. We include the degradation in the mechanical and chemical contributions. The heterogeneous NMC microstructure is considered by representing the material's tensile strength with a Weibull distribution function, which allows to represent complex and non-deterministic crack patterns.

We use our model to provide a comprehensive analysis of mechanical degradation in NMC111 electrodes, including the effect of particle size, C-rate, and depth of charge and discharge. Then, we analyze the influence of the electrode composition (namely, Ni content) on the structural integrity. We use this information to provide design guides for functionally-graded electrodes with high capacity and limited degradation.