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High-Entropy Surface Complex Stabilized LiCoO2 Cathode
DOI:10.1002/aenm.202300147.png)
Abstract
En 中文
Elevating the charge voltage of LiCoO2 increases the energy density of batteries, which is highly enticing in energy storage implementation ranging from portable electronics to e-vehicles. However, hybrid redox reactions at high voltages facilitate oxygen evolution, electrolyte decomposition and irreversible phase change, and accordingly lead to rapid battery capacity decay. Here significantly improved high-voltage cycling stability of Mg-Al-Eu co-doped LiCoO2 is demonstrated. It is found that element co-doping induces a near-surface high-entropy zone, including an innately thin disordered rock-salt shell and a dopant segregation surface. The high-entropy complex can effectively suppress oxygen evolution and near-surface structure deconstruction. The phase change reversibility between O3 and H1-3 and thermal stability of the cathode are greatly enhanced as well. As a result, the co-doped LiCoO2 exhibits a remarkable cycling performance, retaining 86.3% and 72.0% of initial capacity over 800 and 2000 cycles, respectively, with a high cut-off voltage of 4.6 V. The feasible co-doping approach broadens the perspective for the development of stable lithium-ion batteries with high operating voltages.
Keywords:
high-voltage LiCoO2
high-entropy complex
Li-ion batteries
Mg-Al-Eu co-doping
oxygen evolution
Journal
IF:
26
Papers:
1.0W
Citations:
15.7W

