Lithium-rich layered oxides (LRLOs), such as Li1.2Ni0.13Co0.13Mn0.54O2, are gaining attention for their exceptionally high specific capacities (>250 mAh/g) due to anionic redox activity alongside cationic redox processes. Recent studies have shown that optimizing the oxygen lattice structure can achieve capacities as high as 300 mAh/g at low rates (0.05C), nearly doubling the energy density of conventional NMC cathodes. However, challenges such as voltage fade and irreversible oxygen loss remain critical barriers to commercialization.
Surface engineering has emerged as a promising strategy to mitigate these issues. Coating LRLOs with Al2O3 or Li3PO4 has been shown to reduce voltage fade by up to 50% over 100 cycles while maintaining capacities above 240 mAh/g at 0.1C rates. Additionally, doping with elements like Ti or Zr can stabilize the oxygen lattice structure by increasing the activation energy for oxygen evolution from ~1 eV to ~1.5 eV during high-voltage cycling (>4.6 V).
Recent advancements in operando characterization techniques have provided deeper insights into the anionic redox mechanisms in LRLOs. For instance, X-ray absorption spectroscopy (XAS) has revealed that reversible oxygen redox occurs at potentials above ~4 V vs Li+/Li while maintaining structural integrity up to ~4 Kbar pressure during cycling—a key factor in preventing mechanical degradation and improving cycle life beyond >500 cycles with >90% retention.
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