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Co-free gradient lithium-rich cathode for high-energy batteries with optimized cyclability.

Haotian Yang1,2, Lihang Wang1,2, Yuqiang Li1,2

  • 1Institute of Advanced Battery Materials and Devices, College of Materials Science and Engineering, Beijing University of Technology, Beijing 100124, China.

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Cobalt-free, concentration-gradient lithium-rich layered oxides (LLOs) demonstrate remarkable stability for high-energy battery cathodes. This breakthrough minimizes voltage decay and enhances capacity retention, paving the way for advanced energy storage solutions.

Keywords:
battery cathodeconcentration gradientlithium ion batterieslithium-rich layered oxidesredox mechanism

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Energy Storage

Background:

  • Lithium-rich layered oxides (LLOs) are promising for high-energy battery cathodes.
  • Voltage decay due to irreversible reactions at high voltages hinders LLO application.

Purpose of the Study:

  • To investigate the electronic structure of Mn-based LLOs.
  • To design and synthesize novel cobalt-free, concentration-gradient LLOs (CF-CG-LLOs) to overcome voltage decay.

Main Methods:

  • Theoretical study of molecular orbitals in Mn-based Li-rich configurations.
  • Synthesis of cobalt-free concentration-gradient LLOs.
  • Electrochemical testing of pouch cells.

Main Results:

  • Identified stable redox reactions in LiMn6 structures and the disruptive effect of Cobalt.
  • CF-CG-LLOs exhibited exceptional capacity retention over 100 cycles.
  • Achieved ultra-low voltage decay (0.15 mV/cycle) and high Coulombic efficiency (99.86%).

Conclusions:

  • Cobalt removal and concentration gradients are key to stabilizing LLO cathodes.
  • CF-CG-LLOs offer a viable pathway for low-cost, high-energy-density batteries.
  • This approach addresses critical challenges in next-generation battery technology.