Abstract The use of cobalt-free LiNi0.5Mn1.5O4 (LNMO) would provide a great leap forward towards the realization of sustainable lithium-ion batteries. However, the high operating voltage remains to be a great challenge for the cathode/electrolyte stability. Herein, we report a rational material design to address these challenges by carefully tuning the synthesis parameters in order to engineer LNMO crystals with tailored surface facets, providing an exceptional rate capability and improved interfacial stability. The additional introduction of protective TMPOx coatings further enhances the long-term cycling stability, in particular, at elevated cut-off potentials up to 4.95 V, increased temperature of 40 °C, and high dis-/charge rates. As a result of the careful design of the LNMO active material particles, lithium-ion cells employing this material together with Li4Ti5O12 anodes provide an excellent rate capability with 80% of the low-rate capacity at fast dis-/charge rates of 10C combined with highly stable cycling at such high rate, as highlighted by a capacity fading of less than 5% after 1000 cycles.

中文翻译：

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用于高性能锂离子电池的 TMPOx 涂层 LiNi0.5Mn1.5O4 正极的晶体工程

摘要 无钴LiNi0.5Mn1.5O4（LNMO）的使用将为实现可持续锂离子电池提供巨大的飞跃。然而，高工作电压仍然是阴极/电解质稳定性的一大挑战。在此，我们报告了一种合理的材料设计，通过仔细调整合成参数来解决这些挑战，以设计具有定制表面小面的 LNMO 晶体，提供卓越的倍率能力和改善的界面稳定性。额外引入保护性 TMPOx 涂层进一步增强了长期循环稳定性，特别是在截止电位高达 4.95 V、温度升高 40 °C 和高放电/充电速率的情况下。由于 LNMO 活性材料颗粒的精心设计，