Abstract

Mechanical degradation of cathode active material, such as cracks result from volume changes and phase transitions, is one of the main causes of capacity fading in lithium-ion batteries. Understanding the active material’s deformation behavior during cycling and the impact of electrochemical charging on mechanical properties is crucial for understanding the mechanical degradation mechanism and extending battery lifetime.Herein, we investigate the mechanical properties of an electroplated LiCoO2 (LCO) cathode with crystallographic texture as a function of state of charge/discharge. Nanoindentation mapping is used to detect the differences in mechanical behavior between grain boundary and grain interior region. To determine the charged LCO crystals’ mechanical properties and avoid the effects from grain boundaries and air-exposure, in-situ nanoindentation experiments are conducted in a custom mechanical testing system within a scanning electron microscope. Considering the anisotropy of LCO, electron backscatter diffraction analysis is utilized to clarify the crystallographic orientation of the electrodeposited LCO cathode. Our result shows a decreasing tendency in elastic modulus and hardness with state of charge, which can be attributed to the expansion of LCO layered structure. The recovery of mechanical properties after discharge indicates that the changes in measured mechanical properties mainly come from Li deintercalation and intercalation rather than intergranular fracture during cycling. By releasing the relationship between mechanical properties and degree of delithiation, our study provides an insight into modeling studies of electro-chemo-mechanics for electrode materials. Figure 1

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