(Battery Division Postdoctoral Associate Research Award Sponsored by MTI Corporation and the Jiang Family Foundation) Science of Multiphysics Behavior of Si/C Composite Anodes in High-Energy-Density Lithium-Ion Batteries
Authors: Gao Xiang , Xu Jun 
Published: August 2024

The rapidly growing demands on energy storage technologies over the last decade have imposed further requirements for the high energy/power density, safety, and durability of lithium-ion batteries (LIBs). Si/C composite materials have attracted enormous research interest as the most promising candidates for the anodes of next-generation lithium-ion batteries, owing to their high energy density and mechanical buffering property. However, the major disadvantage of materials with ultra-high capacities, such as Si-based materials, is the significant volume change during cycling, which further leads to mechanical and electrochemical degradation. However, a sophisticated and quantitative understanding of the highly electrochemical-mechanical coupling behaviors is still lacking.

A comprehensive computational model is indispensable in the developing process of the excellent performance of anode material due to the low-realizability, inconvenience, and high-cost of experiments, which also provides powerful tools for fabrication guidance of novel Si/C composites designs. Hence, a multiphysics modeling framework is established with a detailed geometric description to quantitatively reveal the underlying governing mechanisms of Si/C composite anode behaviors. We studied the effects of the Si weight percentage, the Si-related particle distribution, the Si-related particle size, the mechanical constraint, and the binder domain gradient on the battery performance regarding the potential behavior, capacity delivery, mechanical stress/strain, Li plating, and polarization evolution. In our study, we used silicon monoxide (SiO) as the Si element source and graphite (Gr) as the C element source. Results discover that an 8-10 wt% of SiO would be an optimal choice regarding capacity delivery and minimizing Li plating under 1C constant current charging condition. Positioning SiO particles near the separator and reducing the sizes of SiO particles are also demonstrated to be beneficial for electrochemical performance with trivial influence on mechanical mismatch. In addition, the mechanical constraint demonstrates a balanced effect on the overall performance of cells and the local behaviors of particles. Our findings also indicate that reducing the proportion of carbon-binder domain (CBD) in the upper domain (near the anode surface) compared to the lower domain (near the current collector) positively influences electrochemical performance, particularly in terms of capacity and Li plating. However, such an arrangement introduces potential risks of mechanical failures and we recommend to incorporate a higher proportion of CBD alongside the SiO particles. Finally, an anode design with a lower CBD proportion in the upper domain exhibits superior rate performance.

This study explores the multiphysics behavior of Si/C anodes material using a comprehensive methodology combining experimental and FEA techniques, systematically revealing the coupling mechanism among various physical fields, as well as providing efficient and powerful tools in the design, development, and evaluation of high energy density lithium-ion batteries.