Anion-redox chemistry is a groundbreaking approach to unlocking higher energy densities in layered oxide cathodes. Materials like Li-rich NMC (Li1.2Ni0.13Co0.13Mn0.54O2) exploit oxygen redox activity to deliver capacities exceeding 300 mAh/g, nearly doubling the theoretical limit of cation-only redox systems. However, this comes with challenges such as oxygen loss and voltage decay during cycling.
Advanced spectroscopic techniques like resonant inelastic X-ray scattering (RIXS) have revealed the complex interplay between anion and cation redox processes in these materials. For example, RIXS data show that oxygen redox contributes ~50% of the total capacity in Li-rich NMC cathodes but also induces lattice distortions that lead to capacity fading over time. Strategies such as surface coating with Al2O3 or doping with Ti have been shown to mitigate these issues effectively.
Recent computational studies using density functional theory (DFT) have identified key descriptors for optimizing anion-redox activity, including metal-oxygen bond covalency and oxygen hole formation energy. These insights have guided the design of new materials like Li2MnO3-LiCoO2 composites, which exhibit stable cycling with less than 0.3 mV/cycle voltage decay after 100 cycles at C/3 rate.
The integration of anion-redox cathodes with solid-state electrolytes is another promising direction, as it minimizes side reactions and enhances safety. Prototype cells using sulfide-based solid electrolytes have demonstrated energy densities of over 400 Wh/kg while maintaining >80% capacity retention after 200 cycles.
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