Concentration dependence of yield stress, thixotropy, and viscoelasticity rheological behavior of lithium-ion battery slurry

The rheological properties of electrode slurry are mainly influenced by the concentration, which further affects the Lithium-ion batteries (LIBs) quality and manufacturing processes. In this work, various methods including steady-state shear, creep, rheological model fitting, hysteresis loop, and small amplitude oscillatory shear (SAOS) measurement were employed to investigate the concentration-dependent rheological behaviors of slurry, in particular its yield stress, thixotropy, and viscoelasticity. Results show that the difference in yield stress obtained from varying methods is observed, in which the yield stresses measured by the SAOS test are closer to the steady-state value due to its advantage that non-destructive property at small deformations only causes minimum disturbance. The improvement of slurry concentration enhances the bonding strength between particles, thereby resulting in an increase of yield stress and thixotropy, and a decrease of the time scale of transient behavior during the creep process. In oscillatory shear measurement, both storage and loss modulus are concentration-dependent, while yielding and strain stiffening corresponding to critical strains exhibit concentration-independent. In addition, the increase in concentration leads to a more pronounced strain stiffening behavior and a lower characteristic frequency as well as a longer relaxation time. Understanding the relationship between concentration and rheological behaviors will be helpful for material design, preparation, and production in different stages.