Mitigating oxygen loss to improve the cycling performance of high capacity cation-disordered cathode materials.
Mitigating oxygen loss to improve the cycling performance of high capacity cation-disordered cathode materials.
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DOI：
10.1038/s41467-017-01115-0
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发表时间：
2017-10-17
影响因子：
16.6
通讯作者：
Ceder G
中科院分区：
文献类型：
--
作者：
Lee J;Papp JK;Clément RJ;Sallis S;Kwon DH;Shi T;Yang W;McCloskey BD;Ceder G
逾渗理论的最新进展表明，阳离子无序锂过量过渡金属氧化物可作为高容量锂离子正极材料。然而，这些材料提供高容量所需的氧氧化还原过程可能会引发氧损失，从而导致在阴极颗粒上形成电阻表面层。我们在这里证明，令人有些惊讶的是，可以使用标准固态方法将氟掺入到无序锂镍钛钼氧化物的本体中，以增加镍含量，并且这种成分修饰在减少氧损失、提高能量密度、平均电压和倍率性能方面非常有效。我们认为，氟掺入带来的阴离子位点价态降低为高容量阳离子无序正极材料的设计提供了重要的机会。锂过量的阳离子无序氧化物作为正极材料的性能取决于循环过程中氧损失的减轻程度。在这里，作者表明，掺入氟是一种有效的策略，可以显着提高此类材料的循环稳定性。
Recent progress in the understanding of percolation theory points to cation-disordered lithium-excess transition metal oxides as high-capacity lithium-ion cathode materials. Nevertheless, the oxygen redox processes required for these materials to deliver high capacity can trigger oxygen loss, which leads to the formation of resistive surface layers on the cathode particles. We demonstrate here that, somewhat surprisingly, fluorine can be incorporated into the bulk of disordered lithium nickel titanium molybdenum oxides using a standard solid-state method to increase the nickel content, and that this compositional modification is very effective in reducing oxygen loss, improving energy density, average voltage, and rate performance. We argue that the valence reduction on the anion site, offered by fluorine incorporation, opens up significant opportunities for the design of high-capacity cation-disordered cathode materials. The performance of lithium-excess cation-disordered oxides as cathode materials relies on the extent to which the oxygen loss during cycling is mitigated. Here, the authors show that incorporating fluorine is an effective strategy which substantially improves the cycling stability of such a material.
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