Presently used experimental techniques for the characterization of tensile and compressive behavior of active layers in lithium-ion batteries have limitations of different kinds. This is particularly true for measurements of compressive properties. Furthermore, the characterizations of time-dependent stress-strain behavior are largely missing. In order to characterize the stress-strain relationship for a dry cathode active layer in lithium-ion batteries, a mechanical testing method is presented that previously has been applied to the testing of optical fibers. The method is based on U-shaped bending of single-side coated aluminum foils, which enables separate measurements of tensile and compressive properties. In particular, the method has clear advantages for measurements of compressive properties in comparison to previously reported techniques. Relaxation experiments are also conducted in order to characterize the time-dependent properties of the dry active layer and to check if these effects could explain the measured hysteresis. It is found that the elastic modulus in compression is significantly larger than the elastic modulus in tension and that the compressive modulus increases with strain level. Contrary, the tensile modulus is approximately independent of strain. Furthermore, hysteresis effects are present at loading-unloading measurements, both for tension and compression. The low values of the measured elastic moduli show that the electrode properties are largely controlled by the binder and carbon additives. It is concluded that the development of particle-particle contacts most likely is the reason for the higher modulus in compression in comparison to tension. The time-dependent effects are significant, primarily for shorter time scales, which explains the relaxation behavior, but they cannot fully explain the hysteresis effects. Most likely non-linear micro-mechanisms do contribute as well.

The effects of electrochemical aging on the mechanical properties of electrodes in lithium-ion batteries are challenging to measure and are largely unknown. Mechanochemical degradation processes occur at different scales within an electrode and understanding the correlation between the degradation of mechanical properties, electrochemical aging, and morphological changes is crucial for mitigating battery performance degradation. This paper explores the evolution of mechanical and electrochemical properties at the layer level in a Ni-rich positive electrode during the initial stages of electrochemical cycling. The investigation involves complementary cross-section analyses aimed at unraveling the connection between observed changes on both macroscopic and microscopic scales. The macroscopic constitutive properties were assessed using a U-shaped bending test method that had been previously developed. The compressive modulus exhibited substantial dependency on both the porous structure and binder properties. It experienced a notable reduction with electrolyte wetting but demonstrated an increase with cycling and aging. During the initial stages of aging, electrochemical impedance spectra revealed increased local resistance near the particle–electrolyte interface. This is likely attributable to factors such as secondary particle grain separation and the redistribution of carbon black. The swelling of particles, compression of the binder phase, and enhanced particle contact were identified as probable factors adding to the elevation of the elastic modulus within the porous layer as a result of cycling.