The applications of Li-ion batteries in the electronics and vehicle industry is increasing at a very rapid pace. This is primarily due to superior properties such as high specific energy storage and power as well as wider operation temperature ranges. Additional potential for improved properties is connected to capacity losses with time and the thereby resulting limitations of lifetime of batteries. The lifetime of a battery is strongly related to the mechanical and chemical degradation of the active material of electrodes during repeated electrochemical reactions at charging and discharging. To identify this phenomenon from a mechanical perspective, the mechanical properties of the electrode active layers should be characterized. Additionally, with the aid of mechanical properties, realistic electro-chemo-mechanical models should be developed to comprehend the mechanisms causing capacity fade.

In the first part of this thesis, macroscopic material properties of the active layers of Li-ion battery electrodes were measured with a unique bending test technique. Contrary to methods previously used; it is capable to overcome the challenges that were encountered in other traditional testing techniques. In papers 1 and 2 this bending test technique (U-shaped bending test), is used to characterize the elastic and viscoelastic behavior of NMC cathodic and graphite anodic active layers, respectively. By using single-sided thin electrode specimens in U-shape bending tests, it was possible to distinguish tensile and compressive elastic and viscoelastic behavior of the electrode active materials. The tensile Young’s moduli of cathodic and anodic active layers are found as 0.73 GPa and 1 GPa, respectively. On the other hand, the compressive Young’s moduli show a stiffening behavior at increasing strains. Stiffnesses between 1.3 GPa and 2.8 GPa for the cathodic active layer, and between 1 GPa and 3.8 GPa for the anodic active layer were recorded. This compressive behavior of the electrode active layers is expected as a result of the porous nature of the materials. In addition, the viscoelastic behavior of the electrode active layers is expressed through Prony series. It was observed that the behavior can be described by a short term (minutes) and a long term (hours, days) relaxation.

In paper 3, a statistical representative volume element is introduced to predict the elastic properties of a dry cathodic electrode active layer. A porous cathodic electrode active layer that is composed of NMC active particles and polymeric binder material with conductive carbon additives is modeled as a face-centered-cubic structure. Several particle-binder and particle-particle interaction conditions are repeated 50 times with random orientations. Based on the statistics for each interaction case, Young’s modulus is estimated. The results show a good agreement with the experimental findings from Paper 1. Furthermore, particle-particle and particle-binder contact force distributions are calculated for 3% of particle swelling. The characteristics of the force distributions are correlated with the typical material failures in the active layer such as particle cracking and binder debonding. The statistical data obtained here are also used to improve an analytical model that was previously derived to estimate the elastic properties of active porous layers. The analytical model, complemented by the statistical results, showed an excellent agreement with the finite element simulations.