Aluminium–sodium targeted co-doping to boost the electrochemical stability of full concentration gradient Ni-rich LiNi0.80Co0.05Mn0.15O2 cathodes

IF 9.4 1区 化学 Q1 CHEMISTRY, PHYSICAL
Kaixu Yang , Zheng Chen , Chunliang Yang , Wei Shi , Yingchang Yang , Chaochuang Yin , Yun Yi , Jianxin Cao
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Abstract

Structural engineering of full concentration gradient (FCG) offers promising prospects for improving the interface and thermal stability of Ni-rich layered cathodes. However, the Ni content in the core of FCG cathode particle is higher than that on the surface, resulting in rapid structural deterioration at the particle core during cycling. To directionally strengthen the structural stability at the cores of FCG cathode particles, this study proposes a dual-cation targeted co-doping strategy that coordinates gradient Al doping with uniform Na doping. Al–Na co-doped FCG Li1-yNayNi0.80Co0.05Mn0.15-xAlxO2 (FNCM–AxNy) cathodes were successfully prepared through a combined in-situ and wet-chemistry method. As confirmed in experimental and theoretical studies, the particle core is structurally stabilized by the directional distribution of Al and Na within the particles, the formation of strong AlO bonds, and the provision of Na pillar ions in the bulk, which alleviate lattice shrinkage and structural collapse of the particles during the cycling process. Moreover, Al–Na co-doping enhances the diffusion kinetics by widening the ion- diffusion channels and reducing the diffusion barriers. Consequently, the capacity retention of the as-prepared FNCM-A0.1N1 cathode (co-doped with 0.1 mol% Al and 1 mol% Na) after 200 cycles at a rate of 1C reached 93 %, considerably outperforming both the pristine cathode (81 %) and the Al-doped cathode (87 %). Our study provides a novel idea to enhance the electrochemical stability by targeting strengthening the structural stability at the particle core of FCG Ni-rich layered cathodes.

Abstract Image

铝钠共掺杂提高全浓度梯度富镍LiNi0.80Co0.05Mn0.15O2阴极的电化学稳定性
全浓度梯度(FCG)结构工程为改善富镍层状阴极的界面和热稳定性提供了广阔的前景。然而,FCG阴极颗粒芯内的Ni含量高于表面的Ni含量,导致循环过程中颗粒芯处结构迅速劣化。为了有方向性地增强FCG阴极颗粒核心处的结构稳定性,本研究提出了一种梯度Al掺杂与均匀Na掺杂相协调的双阳离子定向共掺杂策略。采用原位和湿化学相结合的方法成功制备了Al-Na共掺杂FCG Li1-yNayNi0.80Co0.05Mn0.15-xAlxO2 (FNCM-AxNy)阴极。实验和理论研究证实,Al和Na在颗粒内的定向分布、强AlO键的形成以及体中Na柱离子的提供,减轻了颗粒在循环过程中的晶格收缩和结构崩溃,从而稳定了颗粒核的结构。此外,Al-Na共掺杂通过拓宽离子扩散通道和降低扩散障碍来增强扩散动力学。因此,制备的FNCM-A0.1N1阴极(共掺杂0.1 mol% Al和1 mol% Na)在1C循环200次后的容量保持率达到93%,大大优于原始阴极(81%)和Al掺杂阴极(87%)。本研究为提高富镍层状阴极颗粒核结构稳定性提供了一种新的思路。
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来源期刊
CiteScore
16.10
自引率
7.10%
发文量
2568
审稿时长
2 months
期刊介绍: The Journal of Colloid and Interface Science publishes original research findings on the fundamental principles of colloid and interface science, as well as innovative applications in various fields. The criteria for publication include impact, quality, novelty, and originality. Emphasis: The journal emphasizes fundamental scientific innovation within the following categories: A.Colloidal Materials and Nanomaterials B.Soft Colloidal and Self-Assembly Systems C.Adsorption, Catalysis, and Electrochemistry D.Interfacial Processes, Capillarity, and Wetting E.Biomaterials and Nanomedicine F.Energy Conversion and Storage, and Environmental Technologies
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