Understanding Modulus Variation of the Active Layers of Silicon Composite Electrodes

The variation of the effective modulus of silicon composite electrodes,which is a fundamental feature to analyze the coupled mechanical–electrochemical behavior of Si-based electrodes in high-capacity lithium-ion batteries,remains qualitatively controversial.To clarify the contradictory experimental results,numerical modeling of a representative volume element with silicon particles,carbon-binder domains(CBDs),and pores has been performed for the lithiation process.The key parameters for modulus variation were identified and evaluated.A mesostructure change is proposed to be a crucial mechanism that affects the modulus variation,and silicon softening is another key mechanism.Silicon softening and the decreasing CBD volume fraction collectively result in a decrease in the effective modulus of the composite,whereas an increase in the silicon volume fraction along with a decrease in porosity has the opposite effect.The findings of this work provide an in-depth and fundamental understanding of the mechanical properties of silicon composite electrodes.