High-entropy oxides (HEOs) are emerging as a revolutionary class of cathode materials due to their unique multi-cation composition, which enhances structural stability and electrochemical performance. Recent studies have demonstrated that HEOs like (Mg, Co, Ni, Cu, Zn)O exhibit exceptional capacity retention of over 95% after 500 cycles at 1C rates. The entropy-driven stabilization mechanism allows these materials to operate at high voltages (up to 4.8 V vs. Li/Li+) without significant phase transitions or degradation. This makes HEOs particularly promising for high-energy-density lithium-ion batteries (LIBs).
The tunability of HEOs enables precise control over ionic conductivity and redox activity. For instance, incorporating Cr or Mn into the lattice can increase ionic conductivity by up to 10^-2 S/cm at room temperature, rivaling traditional solid electrolytes. Additionally, the multi-cation environment facilitates multiple redox reactions, enabling capacities exceeding 300 mAh/g in some compositions. This versatility positions HEOs as a platform for next-generation cathodes in both LIBs and sodium-ion batteries (SIBs).
HEOs also exhibit remarkable thermal stability, a critical factor for battery safety. Thermal analysis shows that HEOs maintain structural integrity up to 800°C, significantly higher than layered oxides like NMC (LiNiMnCoO2), which decompose at around 300°C. This property is attributed to the entropy-driven disorder in the crystal lattice, which inhibits oxygen release and reduces the risk of thermal runaway. Such stability is crucial for applications in electric vehicles (EVs) and grid storage systems.
Recent advances in synthesis techniques have further enhanced the performance of HEO cathodes. For example, mechanochemical synthesis methods can produce nanostructured HEOs with particle sizes below 50 nm, leading to improved rate capabilities (>90% capacity retention at 5C). Additionally, doping strategies involving rare-earth elements like La or Ce have been shown to enhance cycling stability by mitigating cation mixing and lattice strain during charge-discharge cycles.
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