The iron-based polyanionic material Na3Fe2(PO4)P2O7 is regarded as an excellent cathode due to its outstanding thermal stability and the three-dimensional(3D) open framework structure with facile sodium-ions transport. However, its...

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Anionic and cationic redox chemistries boost ultrahigh specific capacities of Li‐rich Mn‐based oxides cathodes (LRMO). However, irreversible oxygen evolution and sluggish kinetics result in continuous capacity decay and poor rate performance, restricting the commercial fast‐charging cathodes application for lithium ion batteries. Herein, the local electronic structure of LRMO is appropriately modulated to alleviate oxygen release, enhance anionic redox reversibility, and facilitate Li+ diffusion via facile surface defect engineering. Concretely, oxygen vacancies integrated on the surface of LRMO reduce the density of states of O 2p band and trigger much delocalized electrons to distribute around the transition metal, resulting in less oxygen release, enhancing reversible anionic redox and the MnO6 octahedral distortion. Besides, partially reduced Mn and lattice vacancies synchronously stimulate the electrochemical activity and boost the electronic conductivity, Li+ diffusion rate, and fast charge transfer. Therefore, the modified LRMO exhibits enhanced cyclic stability and fast‐charging capability: a high discharging capacity of 212.6 mAh·g−1 with 86.98% capacity retention after 100 cycles at 1 C is obtained and to charge to its 80%, SOC is shortened to 9.4 min at 5 C charging rate. This work will draw attention to boosting the fast‐charging capability of LRMO via the local electronic structure modulation.

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