How Can the Electrode Influence the Formation of the Solid Electrolyte Interface?

In rechargeable batteries, stable electrode–electrolyte interface (EEI) formation is crucial for achieving high Coulombic efficiency, rate capability, and cycling lifetime. Numerous studies have been conducted on engineering electrolyte components for regulating the EEI. However, the influence of the electrode material on EEI formation has been seldom considered. In this Perspective, we highlight the critical influence of electrode materials on EEI formation, namely the interfacial catalytic mechanism of electrolyte reduction or oxidation by electrodes. We focus on the evolution of the solid electrolyte interface (SEI) on negative electrodes and discuss the direct (defective configurations) and indirect (pore structure) influencing factors promoting catalytic electrolyte reduction. Furthermore, selective regulations of catalytic effects on electrolyte reduction through electrode design are particularly discussed. Finally, challenges and future directions are detailed for obtaining superior SEIs for advanced batteries.