Journal
NPG ASIA MATERIALS
Volume 8, Issue -, Pages -Publisher
NATURE PUBLISHING GROUP
DOI: 10.1038/am.2016.53
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Funding
- JST-CREST 'Phase Interface Science for Highly Efficient Energy Utilization', JST (Japan)
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Layered NaxMeO2 (Me = transition metal) oxides, the most common electrode materials for sodium-ion batteries, fall into different phases according to their stacking sequences. Although the crystalline phase is well known to largely influence the electrochemical performance of these materials, the structure-property relationship is still not fully experimentally and theoretically understood. Herein, a couple consisting of P2-Na0.62Ti0.37Cr0.63O2 and P3-Na0.63Ti0.37Cr0.63O2 materials having nearly the same compositions is reported. The atomic crystal structures and charge compensation mechanism are confirmed by atomic-scale characterizations in the layered P2 and P3 structures, respectively, and notably, the relationship of the crystal structure-electrochemical performance is well defined in the layered P-type structures for the first time in this paper. The electrochemical results suggest that the P2 phase exhibits a better rate capability and cycling stability than the P3 phase. Density functional theory calculations combined with a galvanostatic intermittent titration technique indicates that the P2 phase shows a lower Na diffusion barrier in the presence of multi-Na vacancies, accounting for the better rate capability of the P2 phase. Our results reveal the relationship between the crystal structure and the electrochemical properties in P-type layered sodium oxides, demonstrating the potential for future electrode advancements for applications in sodium-ion batteries.
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