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Integrating Bulk Nb Doping and F Surface Layer to Construct a Robust Li-Rich Mn-Based Layered Cathode with Stable

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This study enhances Li-rich layered oxide cathodes for lithium-ion batteries by combining Nb5+ doping and fluorine modification. This strategy improves structural stability and electrochemical performance, enabling longer battery life.

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Energy Storage

Background:

  • Li-rich layered oxides (LLOs) offer high capacity for next-generation lithium-ion batteries (LIBs).
  • However, LLOs suffer from voltage decay, interfacial instability, and structural degradation during cycling, limiting their practical use.

Purpose of the Study:

  • To develop a synergistic strategy combining Nb5+ doping and surface fluorine modification.
  • To stabilize the crystal and interfacial structures of Li-rich Mn-based layered oxide cathodes.

Main Methods:

  • Synergistic doping with high-valence Nb5+ and surface fluorine modification.
  • Characterization using Rietveld refined XRD, HRTEM/EDS, in situ XRD, DEMS, and EIS.
  • Electrochemical performance testing under various cycling conditions.

Main Results:

  • The modified LLO (M-LLO) exhibited enhanced phase stability and suppressed surface phase transitions.
  • Nb5+ and F- incorporation formed an oxygen vacancy-rich surface layer, improving Li+ diffusion and interfacial stability.
  • M-LLO achieved 89.7% capacity retention after 100 cycles (1 C) and 78.4% after 300 cycles (3 C) with minimal voltage decay (3.3 mV·cycle-1).

Conclusions:

  • The core-surface cooperative engineering strategy effectively stabilizes LLO structures and interfaces.
  • This approach leads to robust, energy-dense cathode materials for advanced LIBs.