Enhancing the performance of Li-rich oxide cathodes through multifunctional surface engineering

IF 8.1 2区 工程技术 Q1 CHEMISTRY, PHYSICAL Journal of Power Sources Pub Date : 2025-03-14 DOI:10.1016/j.jpowsour.2025.236717
Tongxing Lei , Guolin Cao , Xiuling Shi , Bin Cao , Zhiyu Ding , Yu Bai , Junwei Wu , Kaikai Li , Tongyi Zhang
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Abstract

The commercial development of lithium-rich manganese-based cathode materials is limited by severe capacity decay, voltage attenuation and poor rate capability. Herein, a multifunctional surface engineering is successfully applied to improve Li1.2Mn0.54Co0.13Ni0.13O2 materials by a facile method of solution pretreatment followed by high-temperature thermal treatment. Gradient fluorine doping on the near-surface region is demonstrated to induce the higher ratio of Mn3+/Mn4+, the increasing amounts of oxygen vacancies and the decreasing Li+ diffusion energy barrier. Fast-ion-conductivity spinel phase of LiMn2O4 is spontaneously formed on the subsurface and the outmost coating layer that consists of Li3PO4 and LiF is constructed on the surface. The formed heterogeneous layers could not only facilitate Li + rapid transport but also effectively stabilize the surficial structure. The optimal sample is demonstrated to exhibit superior cycling stability and rate capability. The capacity retention after 200 cycles at 1 C is improved from 67.7 % to 91.0 % and the specific capacity at 8 C is increased from 81.9 to 140.8 mAh/g. The voltage attenuation is significantly mitigated, decreasing from 2.02 to 1.05 mV per cycle. The encouraging results may promote the practical application of lithium-rich manganese-based cathode materials in high-energy-density lithium-ion batteries.
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富锂锰基正极材料的商业开发受到严重的容量衰减、电压衰减和速率能力差的限制。本文采用溶液预处理再高温热处理的简便方法,成功应用多功能表面工程技术改进了 Li1.2Mn0.54Co0.13Ni0.13O2 材料。实验证明,在近表面区域的梯度氟掺杂可以提高 Mn3+/Mn4+ 的比例,增加氧空位的数量,降低 Li+ 扩散能垒。在次表面自发形成了快离子导电尖晶石相 LiMn2O4,并在表面构建了由 Li3PO4 和 LiF 组成的最外层涂层。形成的异质层不仅能促进 Li + 的快速传输,还能有效稳定表面结构。实验证明,最佳样品具有优异的循环稳定性和速率能力。在 1 C 下循环 200 次后,容量保持率从 67.7% 提高到 91.0%,8 C 下的比容量从 81.9 mAh/g 提高到 140.8 mAh/g。电压衰减明显减轻,从每循环 2.02 mV 下降到 1.05 mV。这些令人鼓舞的结果可能会促进富锂锰基正极材料在高能量密度锂离子电池中的实际应用。
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来源期刊
Journal of Power Sources
Journal of Power Sources 工程技术-电化学
CiteScore
16.40
自引率
6.50%
发文量
1249
审稿时长
36 days
期刊介绍: The Journal of Power Sources is a publication catering to researchers and technologists interested in various aspects of the science, technology, and applications of electrochemical power sources. It covers original research and reviews on primary and secondary batteries, fuel cells, supercapacitors, and photo-electrochemical cells. Topics considered include the research, development and applications of nanomaterials and novel componentry for these devices. Examples of applications of these electrochemical power sources include: • Portable electronics • Electric and Hybrid Electric Vehicles • Uninterruptible Power Supply (UPS) systems • Storage of renewable energy • Satellites and deep space probes • Boats and ships, drones and aircrafts • Wearable energy storage systems
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