Damage‐Tolerant and Self‐Repairing Web‐Like Borate Type Binder Enable Stable Operation of Efficient Si‐Based Anodes

Abstract Novel binder designs are shown to be fruitful in improving the electrochemical performance of silicon (Si)‐based anodes. However, issues with mechanical damage from dramatic volume change and poor lithium‐ion (Li + ) diffusion kinetics in Si‐based materials still need to be addressed. Herein, an aqueous self‐repairing borate‐type binder (SBG) with a web‐like architecture and high ionic conductivity is designed for Si and SiO electrodes. The 3D web‐like architecture of the SBG binder enables uniform stress distribution, while its self‐repairing ability promotes effective stress dissipation and mechanical damage repair, thereby enhancing the damage tolerance of the electrode. The tetracoordinate boron ions () in the SBG binder boosts the Li transportation kinetics of Si‐based electrodes. Based on dynamic covalent and ionic conductive boronic ester bonds, the diverse requirements of the binder, including uniform stress distribution, self‐repairing ability, and high ionic conductivity, can be met by simple components. Consequently, the proposed straightforward multifunction design strategy for binders based on dynamic boron chemistry provides valuable insights into fabricating high‐performance Si‐based anodes.