A Strong Interfacial Adhesion and High Stress Dissipation Binder for Durable Microsized SiO_x Anodes

Abstract The rapid capacity decay of microsized SiO x anode resulting from large volume change hinders its commercial application. Herein, a polymer binder with strong interfacial adhesion and high stress dissipation is designed to alleviate the volume change of microsized SiO x anode and maintain structural integrity of electrode. The density functional theory calculations (DFT) and X‐ray photoelectron spectroscopy (XPS) reveal that the multifunctional polymeric network enhances interfacial contact between the binder and silicon oxide (SiO x ) particles through gradient hydrogen bonds. Additionally, the designed binder exhibits high mechanical strength and self‐healing function via the synergy of supramolecular and covalent chemistry. The designed binder enables SiO x electrodes to exhibit notable cycling stability and superior rate performances. This work provides valuable insights into the structure‐function relationship of binder for high‐capacity SiO x anodes.