Building Elastic Solid Electrolyte Interphases for Stabilizing Microsized Antimony Anodes in Potassium Ion Batteries

Abstract Alloy anodes composed of microsized particles receive increasing attention recently, which outperform the nanostructured counterparts in both the manufacturing cost and volumetric energy density. However, the pulverization of particles and fracture of solid electrolyte interphase (SEI) during cycling brings about fast capacity degradation. Herein, it is shown how normally considered fragile SEI can become highly elastic through electrolyte chemistry regulation. Compared to the SEI constructed in classic carbonate electrolyte, the atomic force microscopy tests reveal that the one built in ether‐based electrolyte doubles the maximum elastic strain to accommodate the repeated swelling‐contracting. Such an SEI effectively encapsulates the microsized Sb anodes to prevent the capacity loss from particle isolation. Coupled with an intercalation‐assisted alloying reaction mechanism, a sustained capacity of ≈573 mAh g⁻¹ after 180 cycles at 0.1 A g⁻¹ with outstanding initial Coulombic efficiency is obtained, which is among the highest values achieved in K‐ion batteries. This study emphasizes the significance of building robust SEI, which offers the opportunity to enable stable microsized alloy anodes.