Reversible Configurations of 3-Coordinate and 4-Coordinate Boron Stabilize Ultrahigh-Ni Cathodes with Superior Cycling Stability for Practical Li-Ion Batteries

IF 27.4 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Haifeng Yu, Jin Cheng, Huawei Zhu, Ling Chen, Cheng Lian, Yanjie Hu, Honglai Liu, Hao Jiang, Chunzhong Li
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Abstract

Ultrahigh-Ni layered oxide cathodes are the leading candidate for next-generation high-energy Li-ion batteries owing to their cost-effectiveness and ultrahigh capacity. However, the increased Ni content causes larger volume variations and worse lattice oxygen stability during cycling, resulting in capacity attenuation and kinetics hysteresis. Herein, a Li2SiO3-coated Li(Ni0.95Co0.04Mn0.01)0.99B0.01O2 ultrahigh-Ni cathode that well-addresses all the above issues, which is also the first time to realize the real doping of B ions is demonstrated. The as-obtained cathode delivers a reversible capacity of up to 237.4 mAh g−1 (924 Wh kg−1cathode) and a superior capacity retention of 84.2% after 500 cycles at 1C in pouch-type full-cells. Advanced characterizations and calculations verify that the boron-doping is existed in terms of 3-coordinate and 4-coordinate configurations and their high electrochemical reversibility during de-/lithiation, which greatly stabilizes oxygen anions and impedes Ni-ion migration to Li layer. Furthermore, the B-doping engineers the primary particle microstructure for better relaxing the lattice strain and accelerating Li-ion diffusion. This work advances the energy density of cathode materials into the domain of above 900 Wh kg−1, and the concept will inspire more intensive study on ultrahigh-Ni cathodes.

Abstract Image

3 配位硼和 4 配位硼的可逆配置稳定了超高镍阴极,为实用型锂离子电池带来卓越的循环稳定性
超高镍层状氧化物阴极因其成本效益和超高容量而成为下一代高能锂离子电池的主要候选材料。然而,镍含量的增加会导致循环过程中体积变化较大,晶格氧稳定性变差,从而导致容量衰减和动力学滞后。本文展示了一种 Li2SiO3 涂层 Li(Ni0.95Co0.04Mn0.01)0.99B0.01O2 超高镍阴极,很好地解决了上述所有问题,这也是首次实现真正的 B 离子掺杂。这种阴极的可逆容量高达 237.4 mAh g-1(924 Wh kg-1cathode),在袋式全电池中 1C 循环 500 次后,容量保持率高达 84.2%。先进的表征和计算验证了硼掺杂在 3-配位和 4-配位构型中的存在,以及它们在去/硫化过程中的高电化学可逆性,这极大地稳定了氧阴离子,阻碍了镍离子向锂层迁移。此外,B 掺杂还能改善原生粒子的微观结构,从而更好地放松晶格应变并加速锂离子扩散。这项研究将阴极材料的能量密度提高到了 900 Wh kg-1 以上,这一概念将激励人们更加深入地研究超高镍阴极。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
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来源期刊
Advanced Materials
Advanced Materials 工程技术-材料科学:综合
CiteScore
43.00
自引率
4.10%
发文量
2182
审稿时长
2 months
期刊介绍: Advanced Materials, one of the world's most prestigious journals and the foundation of the Advanced portfolio, is the home of choice for best-in-class materials science for more than 30 years. Following this fast-growing and interdisciplinary field, we are considering and publishing the most important discoveries on any and all materials from materials scientists, chemists, physicists, engineers as well as health and life scientists and bringing you the latest results and trends in modern materials-related research every week.
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