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轻微的组成变化诱导的结构无序到有序转变使得层状过渡金属氧化物能够快速存储钠离子。

Slight compositional variation-induced structural disorder-to-order transition enables fast Na storage in layered transition metal oxides.

机构信息

School of Materials, Sun Yat-sen University, Shenzhen, 518107, People's Republic of China.

Spallation Neutron Source Science Center, Dongguan, 523803, People's Republic of China.

出版信息

Nat Commun. 2022 Dec 22;13(1):7888. doi: 10.1038/s41467-022-35597-4.

DOI:10.1038/s41467-022-35597-4
PMID:36550128
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC9780345/
Abstract

The omnipresent Na/vacancy orderings change substantially with the composition that inevitably actuate the ionic diffusion in rechargeable batteries. Therefore, it may hold the key to the electrode design with high rate capability. Herein, the influence of Na/vacancy ordering on Na mobility is demonstrated firstly through a comparative investigation in P2-NaNiMnO and P2-NaNiMnO. The large zigzag Na/vacancy intralayer ordering is found to accelerate Na migration in P2-type NaNiMnO. By theoretical simulations, it is revealed that the Na ordering enables the P2-type NaNiMnO with higher diffusivities and lower activation energies of 200 meV with respect to the P3 one. The quantifying diffusional analysis further prove that the higher probability of the concerted Na ionic diffusion occurs in P2-type NaNiMnO due to the appropriate ratio of high energy ordered Na ions (Na) occupation. As a result, the interplay between the Na/vacancy ordering and Na kinetic is well understood in P2-type layered cathodes.

摘要

Na/空位有序在很大程度上随组成而变化，这不可避免地会影响可充电电池中的离子扩散。因此，它可能是高倍率性能电极设计的关键。本文通过对 P2-NaNiMnO 和 P2-NaNiMnO 的对比研究，首次证明了 Na/空位有序对 Na 迁移率的影响。研究发现，大的锯齿形 Na/空位层内有序促进了 P2 型 NaNiMnO 中的 Na 迁移。通过理论模拟，揭示了 Na 有序使 P2 型 NaNiMnO 的扩散系数更高，且活化能比 P3 型低 200meV。量化的扩散分析进一步证明，由于高能有序 Na 离子（Na）占据的适当比例，P2 型 NaNiMnO 中协同 Na 离子扩散的概率更高。因此，在 P2 型层状阴极中，很好地理解了 Na/空位有序与 Na 动力学之间的相互作用。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/93e6/9780345/983bf2ea0086/41467_2022_35597_Fig5_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/93e6/9780345/fafd7caab610/41467_2022_35597_Fig1_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/93e6/9780345/0aadb5c768cf/41467_2022_35597_Fig2_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/93e6/9780345/6cfcddc50fcb/41467_2022_35597_Fig3_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/93e6/9780345/162707125e6c/41467_2022_35597_Fig4_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/93e6/9780345/983bf2ea0086/41467_2022_35597_Fig5_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/93e6/9780345/fafd7caab610/41467_2022_35597_Fig1_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/93e6/9780345/0aadb5c768cf/41467_2022_35597_Fig2_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/93e6/9780345/6cfcddc50fcb/41467_2022_35597_Fig3_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/93e6/9780345/162707125e6c/41467_2022_35597_Fig4_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/93e6/9780345/983bf2ea0086/41467_2022_35597_Fig5_HTML.jpg

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