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在高层氧化物合成过程中与基本结构单元的重建相结合的阴离子排序

Ming-Jian Zhang^1,2, Gaofeng Teng², Yu-Chen Karen Chen-Wiegart^3,4

¹Sustainable Energy Technologies Department , Brookhaven National Laboratory , Upton , New York 11973 , United States.

Journal of the American Chemical Society

|September 1, 2018

概括

高层氧化物合成包括控制局部结构秩序. 高温对于更好的离子电池阴极在氧化八面体中实现所需的阴极排序至关重要.

科学领域:

材料科学
固态化学
电化学

背景情况:

金属氧化物的特性与基本建筑单元 (BBU) 的局部结构顺序相关.
高过渡金属层氧化物是有前途的离子电池阴极材料.
八面体 (BBU) 中的阴离子排序决定了电化学活性.

研究的目的:

调查BBU是如何从前体继承的,并在合成过程中演变的.
了解LiNi_0.77Mn_0.13Co_0.10O₂从其氧化物中的合成过程.
在分层氧化物形成过程中阐明局部结构秩序的演变.

主要方法:

使用多式现场X射线表征方法.
在从远程到局部个体八面体单位的尺度上研究合成.
使用第一原理计算来证实实时观测.

主要成果:

观察到一个顶层变化, 层层的框架被保留.
确定了Co和Mn相对于Ni的优先氧化,导致NiO₆八面体的局部变化.
在NiO₆中发现了氧气损失和对称性破坏,导致Ni²⁺的移动性和Li-Ni混合 (阴离子乱).
证明高温处理氧化Ni,诱导对称重建和阴离子排序.

结论:

高Ni层氧化物的合成涉及复杂的局部结构演变.
控制NiO₆八面体内的阴极排序是优化阴极性能的关键.
通过合成控制BBU,研究结果为设计功能材料提供了洞察力.

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