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From Inert to Active: Breaking Mott-localization Enables High Na-Storage Performance in Na₄MnFe(PO₄)₃-based Cathode.

Xiao-Tong Wang¹, Zhen-Yi Gu¹, Yan Liu¹

¹State Key Laboratory of Integrated Optoelectronics, MOE Key Laboratory for UV Light-Emitting Materials and Technology, Northeast Normal University, Changchun, Jilin, P. R. China.

Advanced Materials (Deerfield Beach, Fla.)

|April 7, 2026

Summary

This summary is machine-generated.

Researchers activated sodium-ion battery cathodes by breaking Mott localization. This strategy enhances electrochemical activity and enables sustainable energy storage solutions.

Keywords:

Mott‐localization Na4MnFe(PO4)3 cathode sodium‐ion batteries symmetry‐breaking

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Published on: April 17, 2018

Area of Science:

Materials Science
Electrochemistry
Solid-State Chemistry

Background:

Sodium-ion batteries (SIBs) are promising for sustainable energy storage.
Na4MnFe(PO4)3 (NMFP) offers high theoretical voltage and cost-effectiveness but suffers from poor electrochemical activity.
This inactivity is linked to Mott localization in Mn2+ and Fe3+ ions.

Purpose of the Study:

To investigate the cause of poor electrochemical activity in NMFP.
To develop a strategy to overcome Mott localization and enhance NMFP performance.
To establish a new design paradigm for sustainable cathode materials.

Main Methods:

Symmetry-breaking reconstruction of the NMFP structure.
Investigating electronic structure and charge localization.
Analyzing Na+ migration pathways and energy barriers.
Electrochemical performance testing of engineered materials.

Main Results:

Mott localization due to symmetric, half-filled d-orbitals of Mn2+ and Fe3+ was identified as the primary cause of inactivity.
Symmetry-breaking reconstruction successfully promoted electron delocalization and activated multiple redox couples (Mn and Fe).
A novel, low-energy Na+ migration pathway ('Na2 dp Na1') was induced.
The engineered Na4Mn0.5Fe0.5Cr0.5Ti0.5(PO4)3 exhibited a 12.74-fold capacity increase compared to pristine NMFP (138.84 vs. 10.9 mAh g-1).

Conclusions:

Symmetry-breaking is a critical approach for activating Mott-localized states in polyanionic frameworks.
This strategy provides a new paradigm for designing highly redox-active and sustainable cathode materials for SIBs.