High-entropy oxides (HEOs) have emerged as a revolutionary class of cathode precursors, offering unparalleled structural stability and electrochemical performance. Recent studies demonstrate that HEOs like (Mg, Co, Ni, Cu, Zn)O exhibit a capacity retention of 98.5% after 1,000 cycles at 1C rate, far exceeding traditional LiCoO2 (85% retention). The entropy-driven stabilization mechanism reduces phase segregation and suppresses oxygen evolution at high voltages (>4.5 V), making them ideal for next-gen lithium-ion batteries.
The synthesis of HEOs involves advanced techniques such as co-precipitation and spark plasma sintering (SPS), achieving particle sizes below 100 nm with uniform elemental distribution. For instance, (Fe, Mn, Cr, Ni, Co)3O4 spinel HEOs show a specific capacity of 220 mAh/g at 0.1C, with an energy density of ~850 Wh/kg. These materials also exhibit exceptional thermal stability up to 300°C, mitigating safety concerns in high-energy applications.
The role of configurational entropy in HEOs is quantified using DFT calculations and CALPHAD modeling, revealing that entropy stabilization reduces lattice strain by ~30% during cycling. This results in a volumetric expansion of less than 2%, compared to ~10% in conventional cathodes. Such properties make HEOs promising for solid-state batteries, where interfacial stability is critical.
Recent advancements include doping HEOs with rare earth elements like La and Ce to enhance ionic conductivity by up to 40%. For example, La-doped (Ni, Co, Mn)O2 achieves a conductivity of 10^-3 S/cm at room temperature. These materials are also being explored for sodium-ion batteries, showing capacities of ~150 mAh/g with minimal degradation over 500 cycles.
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