Mechanical Failure Mechanism of Silicon-Based Composite Anodes under Overdischarging Conditions Based on Finite Element Analysis

Overdischarge is a severe safety issue that can induce severe mechanical failure of electrode materials in lithium-ion batteries. A considerable volume change of silicon-based composite anodes undoubtedly further aggravates the mechanical failure. However, the mechanical failure mechanism of silicon-based composite anodes under overdischarging conditions still lacks in-depth understanding despite many efforts paid under normal charging conditions. Herein, we have modeled and tracked the mechanical failure evolution of silicon/carbon nanofibers, a typical silicon-based anode, under overdischarging conditions based on the finite element simulation, with derived optimization strategies of optimal Young’s modulus and stable microstructure. The severe contact damage between silicon nanoparticles and carbon nanofibers, which causes larger shedding and breakage risks, has been found to contribute to mechanical failure. To improve the electrode stability, an optimal Young’s modulus interval ranging from ∼75 to ∼150 GPa is found. Furthermore, increasing the embedding depth of silicon nanoparticles in carbon nanofibers has proven to be an effective strategy for improving electrochemical stability due to the faster lithium salt diffusion and more uniform current density distribution, which was further verified by the experimental capacity retention ratio of carbon-coated silicon and silicon/carbon nanofibers (84 vs 75% after 100 cycles). Our results provide meaningful insights into the mechanical failure of silicon-based composite anodes during overdischarging, giving reasonable guidance for electrode safety designs and performance optimization.