Stabilizing Layered‐Type K0.4V2O5 Cathode by K Site Substitution with Strontium for K‐Ion Batteries

Abstract

AbstractDeveloping suitable cathodes with high capacity and high power is challenging for K‐ion batteries. Herein, electrochemical K‐ion storage properties of the layered‐type K0.4V2O5 (KVO) cathode by incorporating divalent strontium ions (Sr2+) into its crystal structure are enhanced. Divalent strontium ions (1.18 Å) are preferentially incorporated into the octahedrally coordinated K (1.38 Å) layers due to the similar ionic size compared to V4+ (0.58 Å). The introduction of 3 mmol of Sr ions in the KVO crystal improves electrical conductivity and reduces K‐ion diffusion energy barriers. In addition, the strong Sr2+ and O2− interaction acts as a structural pillar, suppressing irreversible phase transition during charge–discharge process. Multi‐physics simulations clearly confirm that the K0.34Sr0.03V2O5 (KS3VO) cathode exhibits a more uniform K‐ion distribution and enhanced reactions of K‐ions compared to the KVO cathode at various depths of discharge. As a result, the KS3VO cathode demonstrates improved reversible capacity, cycling stability, and power capability over the KVO cathode in a K‐ion cell. Synchrotron X‐ray analysis reveals how Sr substitution enhances the electrochemical K‐ion storage properties of the KS3VO cathode. In addition, the KS3VO cathode exhibits superior thermal stability and cycling stability in a full cell coupled with a hard carbon anode compared to the KVO cathode.