High-entropy oxides (HEOs) have emerged as a revolutionary class of cathode precursors, offering unparalleled structural stability and electrochemical performance. Recent studies have demonstrated that HEOs such as (Mg, Ni, Co, Cu, Zn)O exhibit a capacity retention of 98.5% after 1,000 cycles at 1C rate, far exceeding traditional layered oxides like NMC811 (85% retention). The entropy-driven stabilization mechanism prevents phase transitions and mitigates oxygen loss, even at high voltages (>4.5V). This makes HEOs ideal for next-generation lithium-ion batteries targeting energy densities beyond 350 Wh/kg.
The synthesis of HEOs involves advanced techniques such as co-precipitation followed by high-temperature annealing (800-1000°C) to achieve uniform cation distribution. Computational studies using density functional theory (DFT) reveal that the configurational entropy of HEOs reduces the formation energy of defects by up to 0.8 eV, enhancing ionic conductivity by a factor of 10 compared to conventional oxides. This is critical for fast-charging applications where ionic transport bottlenecks are prevalent.
HEOs also exhibit exceptional thermal stability, with decomposition temperatures exceeding 300°C compared to ~200°C for NMC811. This is attributed to the synergistic effect of multiple cations occupying octahedral sites, which suppresses exothermic reactions during thermal runaway. Such properties make HEOs suitable for electric vehicle batteries operating in extreme environments.
Recent advancements in doping strategies have further optimized HEO performance. For instance, introducing Al³⁺ into the lattice increases the average voltage plateau to 3.8V while maintaining a specific capacity of ~200 mAh/g. These innovations position HEOs as a cornerstone material for sustainable energy storage systems.
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