Monoclinic Bimetallic Prussian Blue Analog Cathode with High Capacity and Long Life for Advanced Sodium Storage

This is the authors' abstract. We don't add key points for this paper.

Prussian blue analogs (PBAs) are regarded as promising cathode materials for sodium-ion batteries (SIBs), but most of them suffer from an incompatibility between capacity and structural stability. Herein, an innovative disodium ethylenediaminetetraacetate (Na₂EDTA)-assisted hydrothermal method is proposed to synthesize monoclinic Fe-substituted Ni-rich PBA (H-PBA) cathodes for Na-ion storage. The as-designed H-PBA cathode combines the merits of the low strain of a Ni-based PBA framework and the enhanced capacity of N-Fe³⁺/Fe²⁺ redox sites. It can achieve superior sodium-storage performance in terms of capacity, rate capability, and cycle stability. Moreover, ex situ measurements reveal that solid solution (2.0-3.0 V) and phase-transition (3.0-4.0 V) reactions occur during the charge/discharge process to allow almost 1.5 Na⁺ storage in the H-PBA lattice. Meanwhile, the H-PBA//NaTi₂(PO₄)₃@C full cell also delivers remarkable electrochemical properties. Prospectively, this work would promote the practical application of SIBs in grid-scale electric energy storage.