Enhance cycle life of Na3.32Fe2.34(P2O7)2 cathode by pillar cations

As a safe and sustainable cathode material for reversible Na-ion storage, the electrochemical performance of Na3.32Fe2.34(P2O7)2 with high operational safety can be enhanced via ion-doping engineering strategy. However, the rationale behind has remained unclear. In this study, we partially replace the Na+ and Fe2+ cations with K+ and Mg2+, respectively, where the K+ and Mg2+ dopants serve as pillars to support the crystallographic framework and thus reduce potential hysteresis. It is found that, compared to K doping at the Na site, Mg doping at the Fe site contributes to a more stable crystal structure and renders higher rate capability and cycling stability due to the inhibition of Fe migration and the reduction of structural disorder. The cation pillar strategy reported herein may shed light on enhancing cycling performance of other cathode materials for stable storage of not only Na ions but also other metals.