Anion-redox chemistry has unlocked unprecedented capacities in cathode materials by enabling reversible oxygen redox alongside traditional transition metal redox. Materials like Li-rich layered oxides (e.g., Li1.2Ni0.13Co0.13Mn0.54O2) have demonstrated capacities exceeding 300 mAh/g, nearly doubling the theoretical limit of conventional cathodes. However, this comes at the cost of voltage hysteresis (>0.5 V) and oxygen evolution during cycling, which degrade long-term performance.
Recent advances in doping strategies have mitigated these issues by stabilizing the oxygen lattice during redox reactions. For example, doping Li-rich oxides with elements like Ru or Mo has reduced voltage hysteresis to <0.3 V while maintaining capacities above 250 mAh/g after 100 cycles. These dopants act as electronic reservoirs, facilitating charge compensation without destabilizing the crystal structure or promoting oxygen loss during deep discharge states.
Operando characterization techniques such as X-ray absorption spectroscopy (XAS) and neutron diffraction have provided critical insights into the mechanisms of anion redox behavior in these materials at atomic resolution . Studies reveal that reversible oxygen redox occurs primarily through localized electron holes on oxygen anions rather than delocalized band states , offering a pathway to design more stable high-capacity cathodes . These findings are guiding the development of new materials with optimized anion-redox activity .
Despite progress , challenges persist in achieving long-term cycle life without compromising energy density . Strategies such as surface coatings , nanostructuring , and hybrid anion-cation redox systems are being explored to address these limitations while pushing the boundaries of cathode performance .
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