Design and tailoring of carbon-Al2O3 double coated nickel-based cation-disordered cathodes towards high-performance Li-ion batteries

材料科学 X射线光电子能谱 阴极 氧化还原 氧化物 化学工程 插层(化学) 涂层 X射线吸收光谱法 无机化学 纳米技术 吸收光谱法 物理化学 化学 冶金 工程类 物理 量子力学
作者
Zhenlu Yu,He Huang,Yunjian Liu,Xingyu Qu,Yu Zhou,Aichun Dou,Mingru Su,Hong‐Hui Wu,Liang Zhang,Kehua Dai,Zhanhu Guo,Tao Wan,Mengyao Li,Dewei Chu
出处
期刊:Nano Energy [Elsevier BV]
卷期号:96: 107071-107071 被引量:33
标识
DOI:10.1016/j.nanoen.2022.107071
摘要

Li-excess cation-disordered oxide cathodes have attracted increasing interests owing to their high energy density originated from cumulative cationic & anionic redox activity. In particular, Ni-based cation-disordered oxides exhibit high theoretical capacity for 2 e− reactions of Ni2+/Ni4+, while the severe overlapping between Ni 3d and O 2p orbitals restricts Ni redox capacity and unstable O redox deteriorates the cycling performance. Benefiting from advanced data mining and high-throughput theoretical calculations technology, we demonstrated that the capacity and cycling performance of Ni-based cation-disordered oxide can be synergically enhanced by carbon/Al2O3 double coating and partial Al3+ substitution. The synergistic mechanism is unveiled via X-ray photoelectron spectroscopy (XPS) and soft X-ray absorption spectroscopy (XAS) characterization together with first-principles calculations. It is confirmed that carbon coating increases the capacity by promoting the formation of peroxo-like species, which boosts O redox activity. Partial intercalating Al3+ enhances the Ni redox reaction by shortening the band overlap between Ni and O. Furthermore, Al2O3 coating and Al3+ doping improved the cycling stability of the cathode material owing to the shielding effect on side reaction and more stable O lattice. This synergistic strategy with nano-coating layer provides a promising pathway to accelerate the discovery of high-energy cation-disordered oxides based cathode materials.
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