An Improved Experiment for Measuring Lithium Concentration-Dependent Material Properties of Graphite Composite Electrodes.

The in situ curvature measurement of bilayer beam electrodes is widely used to measure the lithium concentration-dependent material properties of lithium-ion battery electrodes, and further understand the mechano-electrochemical coupling behaviors during electrochemical cycling. The application of this method relies on the basic assumption that lithium is uniformly distributed along the length and thickness of the curved active composite layer. However, when the electrode undergoes large bending deformation, the distribution of lithium concentration in the electrolyte and active composite layer challenges the reliability of the experimental measurements. In this paper, an improved experiment for simultaneously measuring the partial molar volume and the elastic modulus of the graphite composite electrode is proposed. The distance between the two electrodes in the optical electrochemical cell is designed and graphite composite electrodes with four different thickness ratios are measured. The quantitative experimental data indicate that the improved experiment can better satisfy the basic assumptions. The partial molar volume and the elastic modulus of the graphite composite electrode evolve nonlinearly with the increase of lithium concentration, which are related to the phase transition of graphite and also affected by the other components in the composite active layer. This improved experiment is valuable for the reliable characterization of the Li concentration-dependent material properties in commercial electrodes, and developing next-generation lithium batteries with more stable structures and longer lifetimes.