Unveiling the Interplay Between Silicon and Graphite in Composite Anodes for Lithium‐Ion Batteries

Si provides an effective approach to achieving high‐energy batteries owing to its high energy density and abundance. However, the poor stability of Si requires buffering with graphite particles when used as anodes. Currently, commercial lithium‐ion batteries with Si/graphite composite anodes can provide a high energy density and are expected to replace traditional graphite‐based batteries. The different lithium storage properties of Si and graphite lead to different degrees of lithiation and chemical environments for this composite anode, which significantly affects the performance of batteries. Herein, the interplay between Si and graphite in mechanically mixed Si/graphite composite anodes is emphasized, which alters the lithiation sequence of the active materials and thus the cycling performance of the battery. Furthermore, performance optimization can be achieved by changing the intrinsic properties of the active materials and external operating conditions, which are summarized and explained in detail. The investigation of the interplay based on Si/graphite composite anodes lays the foundation for developing long‐life and high‐energy batteries. The abovementioned experimental methods provide logical guidance for future research on composite electrodes with multiple active materials. Silicon/graphite composite anodes are considered the most commercially promising, but the interplay between the different materials affects battery performance. Here, the microstructure, lithiation behavior, and interplay between the two after mixing are elaborated from the microscale to the macroscale. Improvement measures are summarized from the perspective of interplay, and future development directions are envisioned. An in‐depth study of this interplay is highly important for battery development.