Regularly Arranged Micropore Architecture Enables Efficient Lithium-Ion Transport in SiOx/Artificial Graphite Composite Electrode

Abstract

To enhance the electrochemical performance of lithium-ion battery anodes with higher silicon content, it is essential to engineer their microstructure for better lithium-ion transport and mitigated volume change as well. Herein, we suggest an effective approach to control the micropore structure of silicon oxide (SiOx)/artificial graphite (AG) composite electrodes using a perforated current collector. The electrode features a unique pore structure, where alternating high-porosity domains and low-porosity domains markedly reduce overall electrode resistance, leading to a 20% improvement in rate capability at a 5C-rate discharge condition. Using microstructure-resolved modeling and simulations, we demonstrate that the patterned micropore structure enhances lithium-ion transport, mitigating the electrolyte concentration gradient of lithium-ion. Additionally, perforating current collector with a chemical etching process increases the number of hydrogen bonding sites and enlarges the interface with the SiOx/AG composite electrode, significantly improving adhesion strength. This, in turn, suppresses mechanical degradation and leads to a 50% higher capacity retention. Thus, regularly arranged micropore structure enabled by the perforated current collector successfully improves both rate capability and cycle life in SiOx/AG composite electrodes, providing valuable insights into electrode engineering.