Structural evolution of the cathode during cycling plays a vital role in the electrochemical performance of sodium‐ion batteries. A strategy based on engineering the crystal structure coupled with chemical substitution led to the design of the layered P2@P3 integrated spinel oxide cathode Na_0.5Ni_0.1Co_0.15Mn_0.65Mg_0.1O₂, which shows excellent sodium‐ion half/full battery performance. Combined analyses involving scanning transmission electron microscopy with atomic resolution as well as in situ synchrotron‐based X‐ray absorption spectra and in situ synchrotron‐based X‐ray diffraction patterns led to visualization of the inherent layered P2@P3 integrated spinel structure, charge compensation mechanism, structural evolution, and phase transition. This study provides an in‐depth understanding of the structure‐performance relationship in this structure and opens up a novel field based on manipulating structural evolution for the design of high‐performance battery cathodes.

中文翻译：

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为高性能钠离子电池操纵分层的P2 @ P3集成尖晶石结构演变。

循环过程中阴极的结构演变在钠离子电池的电化学性能中起着至关重要的作用。基于对晶体结构进行工程设计并结合化学取代的策略，导致了层状P2 @ P3集成尖晶石氧化物阴极的设计Na _0.5 Ni _0.1 Co _0.15 Mn _0.65 Mg _0.1 O ₂，它具有出色的钠离子半/全电池性能。结合具有原子分辨率的扫描透射电子显微镜，原位基于同步加速器的X射线吸收光谱和原位基于同步加速器的X射线衍射图谱的组合分析，可以看到固有的分层P2 @ P3集成尖晶石结构，电荷补偿机理，结构演变和相变。这项研究提供了对这种结构中结构与性能关系的深入了解，并为操纵高性能电池正极设计开辟了一个基于操纵结构演变的新领域。