K_0.83V₂O₅: A New Layered Compound as a Stable Cathode Material for Potassium-Ion Batteries

Recently, potassium-ion batteries (PIBs) are being actively investigated. The development of PIBs calls for cathode materials with a rigid framework, reversible electrochemical reactivity, and a high amount of extractable K ions, which is extremely challenging due to the large size of potassium. Herein, a new layered compound K_0.83V₂O₅ is reported as a potential cathode material for PIBs. It delivers an initial depotassiation capacity of 86 mAh g^-1 and exhibits a reversible capacity of 90 mAh g^-1 with a high redox potential of 3.5 V (vs K⁺/K) and a capacity retention of more than 80% after 200 cycles. Experimental investigations combined with theoretical calculation indicate that depotassiation-potassiation is accommodated by contraction-expansion of the interlayer spacing along with unpuckering-puckering of the layers. Additionally, the calculated electronic structure suggests the (semi)metallic feature of K_xV₂O₅ (0 < x ≤ 0.875) and K-ion transport in the material is predicted to be one-dimensional with the experimentally estimated chemical diffusion coefficient in the order of 10^-15-10^-12 cm² s^-1. Finally, a K-ion full cell consisting of the K_0.83V₂O₅ cathode and a graphite anode is demonstrated to deliver an energy density of 136 Wh kg^-1. This study will provide insights for further designing novel layered cathodes with high K-ion content for PIBs.