Lithium-rich layered oxides (LRLOs) are gaining attention due to their ability to utilize both cationic and anionic redox reactions for charge storage. By leveraging oxygen redox activity, LRLOs achieve specific capacities exceeding 300 mAh/g, far beyond the theoretical limits of conventional cathodes. Recent studies have demonstrated that doping with elements like Ru or Ir can stabilize oxygen redox activity while minimizing oxygen loss during cycling. For example, a Ru-doped LRLO exhibited a capacity retention of 85% after 200 cycles at 0.2C compared to only 60% for undoped counterparts.
The fundamental mechanisms underlying anionic redox remain poorly understood but are critical for optimizing LRLO performance. Advanced characterization techniques such as operando X-ray absorption spectroscopy (XAS) and resonant inelastic X-ray scattering (RIXS) have revealed that oxygen redox involves reversible formation and dissociation of peroxo-like (O2)^n- species. These insights have guided the design of new LRLO compositions with improved reversibility and reduced voltage hysteresis (<50 mV). Computational studies further suggest that controlling the local coordination environment around oxygen atoms can enhance redox stability by up to 30%.
Despite their high capacities, LRLOs suffer from voltage fade due to structural rearrangements during cycling. Recent breakthroughs in surface engineering have shown promise in mitigating this issue; for instance, coating LRLOs with Al2O3 nanoparticles reduced voltage fade by over 50% after 100 cycles while maintaining a specific capacity above 250 mAh/g at C/5 rate.
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