Computational Design and Preparation of Cation‐Disordered Oxides for High‐Energy‐Density Li‐Ion Batteries
Computational Design and Preparation of Cation‐Disordered Oxides for High‐Energy‐Density Li‐Ion Batteries
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DOI：
10.1002/aenm.201600488
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发表时间：
2016-08
影响因子：
27.8
通讯作者：
A. Urban;Ian L. Matts;A. Abdellahi;G. Ceder
中科院分区：
文献类型：
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作者：
A. Urban;Ian L. Matts;A. Abdellahi;G. Ceder
阳离子无序锂过量金属氧化物近年来作为一种有前途的新型高能密度锂离子电池正极材料出现，但无序材料的探索一直受到其广阔和未开发的成分空间的阻碍。本研究提出了一种鉴定稳定阳离子紊乱岩盐的实用方法。本文证明了利用特殊的准随机结构的有效方法能够正确地预测阳离子有序强度，与精确的蒙特卡罗模拟和实验观察相一致。本研究将此方法应用于三元氧化物的组成空间，分子式单位为LiA0.5B0.5O2 （A， B：过渡金属），发现了一种以前未知的阳离子无序结构LiCo0.5Zr0.5O2，这可能成为一类新的阳离子无序正极材料的基础。这一计算预测通过固态合成和随后的粉末X射线衍射表征得到了实验证实，证明了计算筛选大组成空间以加速材料发现的潜力。
Cation‐disordered lithium‐excess metal oxides have recently emerged as a promising new class of high‐energy‐density cathode materials for Li‐ion batteries, but the exploration of disordered materials has been hampered by their vast and unexplored composition space. This study proposes a practical methodology for the identification of stable cation‐disordered rocksalts. Here, it is established that the efficient method, which makes use of special quasirandom structures, correctly predicts cation‐ordering strengths in agreement with accurate Monte‐Carlo simulations and experimental observations. By applying the approach to the composition space of ternary oxides with formula unit LiA0.5B0.5O2 (A, B: transition metals), this study discovers a previously unknown cation‐disordered structure, LiCo0.5Zr0.5O2, that may function as the basis for a new class of cation‐disordered cathode materials. This computational prediction is confirmed experimentally by solid‐state synthesis and subsequent characterization by powder X‐ray diffraction demonstrating the potential of the computational screening of large composition spaces for accelerating materials discovery.