A New Strategy for High-Voltage Cathodes for K-Ion Batteries: Stoichiometric KVPO4F
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- A New Strategy for High-Voltage Cathodes for K-Ion Batteries: Stoichiometric KVPO4F
- Kim, Haegyeom; Seo, Dong-Hwa; Bianchini, Matteo; Clement, Raphaele J.; Kim, Hyunchul; Kim, Jae Chul; Tian, Yaosen; Shi, Tan; Yoon, Won-Sub; Ceder, Gerbrand
- Issue Date
- WILEY-V C H VERLAG GMBH
- ADVANCED ENERGY MATERIALS, v.8, no.26, pp.1801591
- The exploration of high-energy-density cathode materials is vital to the practical use of K-ion batteries. Layered K-metal oxides have too high a voltage slope due to their large K+-K+ interaction, resulting in low specific capacity and average voltage. In contrast, the 3D arrangement of K+, with polyanions separating them, reduces the strength of the effective K+-K+ repulsion, which in turn increases specific capacity and voltage. Here, stoichiometric KVPO4F for use as a high-energy-density K-ion cathode is developed. The KVPO4F cathode delivers a reversible capacity of approximate to 105 mAh g(-1) with an average voltage of approximate to 4.3 V (vs K/K+), resulting in a gravimetric energy density of approximate to 450 Wh kg(-1). During electrochemical cycling, the KxVPO4F cathode goes through various intermediate phases at x = 0.75, 0.625, and 0.5 upon K extraction and reinsertion, as determined by ex situ X-ray diffraction characterization and ab initio calculations. This work further explains the role of oxygen substitution in KVPO4+xF1-x: the oxygenation of KVPO4F leads to an anion-disordered structure which prevents the formation of K+/vacancy orderings without electrochemical plateaus and hence to a smoother voltage profile.
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