阴极
材料科学
阳极
氧化物
电化学
密度泛函理论
纳米技术
异质结
离子
插层(化学)
结构稳定性
化学物理
化学工程
电极
无机化学
物理化学
光电子学
化学
计算化学
有机化学
冶金
结构工程
工程类
作者
Yao Xiao,Hongrui Wang,Haiyan Hu,Yanfang Zhu,Shi Li,Jiayang Li,Xiongwei Wu,Shulei Chou
标识
DOI:10.1002/adma.202202695
摘要
It is still very urgent and challenging to simultaneously develop high-rate and long-cycle oxide cathodes for sodium-ion batteries (SIBs) because of the sluggish kinetics and complex multiphase evolution during cycling. Here, the concept of accurately manipulating structural evolution and formulating high-performance heterostructured biphasic layered oxide cathodes by local chemistry and orbital hybridization modulation is reported. The P2-structure stoichiometric composition of the cathode material shows a layered P2- and O3-type heterostructure that is explicitly evidenced by various macroscale and atomic-scale techniques. Surprisingly, the heterostructured cathode displays excellent rate performance, remarkable cycling stability (capacity retention of 82.16% after 600 cycles at 2 C), and outstanding compatibility with hard carbon anode because of the integrated advantages of intergrowth structure and local environment regulation. Meanwhile, the formation process from precursors during calcination and the highly reversible dynamic structural evolution during the Na+ intercalation/deintercalation process are clearly articulated by a series of in situ characterization techniques. Also, the intrinsic structural properties and corresponding electrochemical behavior are further elucidated by the density of states and electron localization function of density functional theory calculations. Overall, this strategy, which finely tunes the local chemistry and orbitals hybridization for high-performance SIBs, will open up a new field for other materials.
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