Mansley Zachary R, Millares Marie F, Kazanjian Olivia, Luo Jessica, Takeuchi Esther S, Marschilok Amy C, Bai Jianming, Yan Shan, Takeuchi Kenneth J, Zhu Yimei
Interdisciplinary Science Department, Brookhaven National Laboratory, Upton, New York 11973, United States.
Department of Condensed Matter Physics and Materials Science, Brookhaven National Laboratory, Upton, New York 11973, United States.
Nano Lett. 2025 Jul 30;25(30):11594-11600. doi: 10.1021/acs.nanolett.5c02373. Epub 2025 Jul 16.
High-entropy layered oxides (HELOs) hold great promise as battery cathodes, yet a fundamental understanding regarding the relationships among their atomic composition, crystallographic phase, and structural order remains lacking. In particular, the characterization of short-range order (SRO) is technically challenging but essential, as SRO directly impacts cation distributions within the lattice and thereby governs lithium-ion diffusion pathways. Here we extend beyond the predominantly studied cubic systems and identify diffuse scattering signatures of SRO in a high-entropy layered oxide with 3 symmetry. Through investigation of four lithiated Mn, Ni, Fe, Co, and Al HELOs of the same composition prepared under different annealing conditions, we determine the relationship among crystallinity, antisite mixing, and SRO and electrochemically measured lithium diffusion behavior. We reveal that SRO achieved through higher annealing temperatures and shorter durations promotes more facile Li transport.
高熵层状氧化物（HELOs）作为电池阴极具有巨大潜力，但目前仍缺乏对其原子组成、晶体相和结构有序性之间关系的基本理解。特别是，短程有序（SRO）的表征在技术上具有挑战性，但至关重要，因为SRO直接影响晶格内的阳离子分布，从而控制锂离子扩散途径。在这里，我们超越了主要研究的立方体系，确定了具有三方对称性的高熵层状氧化物中SRO的漫散射特征。通过研究在不同退火条件下制备的四种相同组成的锂化Mn、Ni、Fe、Co和Al的HELOs，我们确定了结晶度、反位混合和SRO与电化学测量的锂扩散行为之间的关系。我们发现，通过更高的退火温度和更短的持续时间实现的SRO促进了更易的锂传输。
