Measuring microscale mechanical properties of PVdF binder phase and the binder-particle interface using micromechanical testing

In this study, we developed a robust methodology for extracting the mechanical properties of individual components in complex systems such as Li-ion battery electrodes and provided quantitative values that can be used as input for modelling and lifetime estimation of Li-ion batteries. We employed micromechanical testing techniques, including micropillar compression, microcantilever bending, and nanoindentation, to measure the mechanical properties of the PVdF binder phase in the active layer. We discovered that nanoindentation tends to overestimate the modulus due to uncertainty associated with the test volume and initial large compression strains, while the micropillar compression technique provides more accurate modulus data with a narrower spread. Additionally, the yield stress of the binder phase can be evaluated using micropillar compression. Our obtained modulus values were in the range of 2.5–4.4 GPa, and the yield stress was in the range of 162–270 MPa. By microcantilever bending tests, we determined that the binder–particle interface often fails before the binder itself, suggesting that the interface significantly influences the failure mechanics. Overall, our results indicate that the microcantilever bending tests provide moduli estimates that agree with those obtained from micropillar compression tests. We also qualitatively examined the binder-particle and binder-current collector interfaces, further emphasising the significance of our methodology and the obtained quantitative values.