Anionic redox chemistry in layered oxide cathodes has emerged as a groundbreaking approach to achieve ultra-high energy densities exceeding 1000 Wh/kg. Materials like Li-rich Li1.2Ni0.13Co0.13Mn0.54O2 exploit oxygen redox activity alongside cationic redox reactions to deliver capacities above 300 mAh/g at C/10 rates. However, this process is often accompanied by oxygen evolution and structural instability during cycling. Advanced characterization techniques such as operando X-ray absorption spectroscopy have revealed that surface coatings like Al2O3 can suppress oxygen loss by forming stable interfaces.
The integration of anionic redox with cation-disordered rock-salt structures has shown promise in mitigating voltage fade and hysteresis issues observed in Li-rich cathodes. For example, Li1.3Nb0.3Mn0.4O2 exhibits a reversible capacity of ~250 mAh/g with minimal voltage decay over 100 cycles at C/5 rate due to its unique cation disorder that stabilizes oxygen redox activity.
Challenges remain in optimizing the trade-off between energy density and cycle life for anionic redox-activated cathodes. Sulfide-Based Solid-State Cathodes,Sulfide-based solid-state electrolytes paired with high-capacity cathodes like LiNi0.8Co0.1Mn0.1O2 (NCM811) are revolutionizing solid-state battery technology due to their high ionic conductivities exceeding 10^-2 S/cm at room temperature.
Recent studies have demonstrated that sulfide-based cathodes can achieve energy densities above 400 Wh/kg when combined with lithium metal anodes.,The interface stability between sulfide electrolytes and cathodes remains a critical challenge.
Advanced interfacial engineering strategies such as atomic layer deposition (ALD) coatings have been shown to reduce interfacial resistance by up to 70%. Single-Crystal NCM Cathodes,Single-crystal NCM (LiNi_xCo_yMn_zO2) cathodes are gaining attention for their superior mechanical stability and reduced cracking compared to polycrystalline counterparts.
Recent research has shown that single-crystal NCM811 can achieve a capacity retention of ~92% after 1000 cycles at C/3 rate due to its robust structure.,The synthesis of single-crystal NCM requires precise control over sintering temperatures and times.
Despite their advantages single-crystal NCM cathodes face challenges related to cost scalability. Halide-Based Cathode Materials,Halide-based cathode materials such as Li3YCl6 are emerging as promising candidates for all-solid-state batteries due to their high ionic conductivities (~10^-4 S/cm) and wide electrochemical stability windows (>4V)."
Recent studies have demonstrated that halide-based cathodes can achieve specific capacities exceeding 150 mAh/g at C/5 rates while maintaining excellent cyclability over hundreds of cycles.
The use of halides also enables compatibility with lithium metal anodes without significant dendrite formation or interfacial degradation.
However challenges remain in optimizing the electronic conductivity of halide-based materials which is currently below ~10^-6 S/cm limiting their rate performance.
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