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Surface Gradient Doping Enables High-Capacity and Long-Life Manganese-Based Prussian Blue Cathodes for Sodium-Ion
Hong Kang1, Lifeng Wang2, Ling Li1
1Hefei National Research Center for Physical Sciences at the Microscale, Department of Materials Science and Engineering, University of Science and Technology of China, Hefei, Anhui, China.
Angewandte Chemie (International Ed. in English)
|May 20, 2026
Summary
Gradient surface doping with copper stabilizes manganese-based Prussian blue analogues (MnPBAs) for sodium-ion batteries (SIBs). This approach enhances cycling stability and capacity retention, paving the way for durable SIB cathodes.
Area of Science:
- Materials Science
- Electrochemistry
- Energy Storage
Background:
- Manganese-based Prussian blue analogues (MnPBAs) are promising cathodes for sodium-ion batteries (SIBs) due to their favorable electrochemical properties and cost-effectiveness.
- However, MnPBAs suffer from capacity decay caused by Jahn-Teller distortion, lattice strain, and manganese dissolution during cycling, limiting their practical application.
Purpose of the Study:
- To develop a stabilized MnPBA cathode material for sodium-ion batteries with enhanced capacity retention and cycle life.
- To investigate the effect of surface copper concentration-gradient doping on the structural stability and electrochemical performance of MnPBAs.
Main Methods:
- A two-step coprecipitation strategy was employed to synthesize copper-doped MnPBAs with a surface concentration gradient (Cu@MnPBA).
- The structural and electrochemical properties of Cu@MnPBA were characterized using various analytical techniques and battery performance testing.
Main Results:
- The Cu@MnPBA material exhibited a unique surface architecture with a ~200 nm Cu-gradient layer and a ~10 nm Cu-rich amorphous outer layer.
- This gradient doping effectively suppressed Jahn-Teller distortion, reduced lattice strain, inhibited Mn dissolution, and improved Na+ surface diffusion.
- Cu@MnPBA demonstrated a high specific capacity of 143.9 mAh g-1 and retained 78% capacity after 500 cycles at 100 mA g-1.
- In a pouch cell configuration with a hard carbon anode, the system maintained 75% capacity after 3000 cycles.
Conclusions:
- Gradient surface doping is an effective strategy to enhance the structural integrity and electrochemical performance of MnPBAs for SIBs.
- The developed Cu@MnPBA cathode exhibits exceptional durability and high capacity, making it suitable for practical sodium-ion battery applications.
- This research provides a valuable design principle for developing next-generation Prussian blue cathode materials for high-performance energy storage systems.
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