Understanding improved stability of Co-free Ni-rich single crystal cathode materials by combined bulk and surface modifications

IF 21.1 1区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Materials Today Pub Date : 2024-05-01 DOI:10.1016/j.mattod.2024.02.003
Qiang Deng , Qimeng Zhang , Youqi Chu , Yunkai Xu , Shunzhang You , Kevin Huang , Chenghao Yang , Jun Lu
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Abstract

Co-free Ni-rich single crystal LiNixMn1-xO2 (x ≥ 0.6) (denoted as SCNM) have been actively studied as a candidate cathode for high energy density and low-cost lithium-ion batteries (LIBs). However, their practical use in LIBs is significantly hindered by their poor chemo-mechanical stability and short cycle life. Herein, we show much improved structural stability and cycle life by bulk and surface modifications of SCNM. We show strong evidence that bulk Ti-doping and gradient Nb-doping are effective in stabilizing lattice oxygen and suppressing detrimental phase transformations, while LiTi2-xNbx(PO4)3 (LTNP) surface coating protects SCNM from reacting with liquid electrolyte and promotes formation of thin and robust interphase layers. As a result, LTNP-modified SCNM achieves an excellent electrochemical performance with 87.2% capacity retention after 100 cycles at high voltage of 4.4 V. This work demonstrates a new approach to stabilize lattice oxygen of Co-free and Ni-rich cathodes and their interfaces with liquid electrolytes, thus contributing to the development of high-energy–density LIBs.

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了解通过结合块体和表面改性提高无钴富镍单晶阴极材料的稳定性
作为高能量密度和低成本锂离子电池(LIB)的候选正极,无钴富镍单晶 LiNixMn1-xO2(x ≥ 0.6)(简称 SCNM)已被积极研究。然而,它们在锂离子电池中的实际应用却因化学机械稳定性差和循环寿命短而受到严重阻碍。在此,我们展示了通过对 SCNM 进行块体和表面改性而大大提高的结构稳定性和循环寿命。我们的研究有力地证明,钛掺杂和铌梯度掺杂能有效稳定晶格氧并抑制有害的相变,而 LiTi2-xNbx(PO4)3 (LTNP) 表面涂层能保护 SCNM 不与液态电解质发生反应,并促进形成薄而坚固的相间层。因此,LTNP 改性 SCNM 实现了优异的电化学性能,在 4.4 V 的高压下循环 100 次后,容量保持率达到 87.2%。这项工作展示了一种稳定无钴和富镍阴极晶格氧及其与液态电解质界面的新方法,从而促进了高能量密度 LIB 的开发。
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来源期刊
Materials Today
Materials Today 工程技术-材料科学:综合
CiteScore
36.30
自引率
1.20%
发文量
237
审稿时长
23 days
期刊介绍: Materials Today is the leading journal in the Materials Today family, focusing on the latest and most impactful work in the materials science community. With a reputation for excellence in news and reviews, the journal has now expanded its coverage to include original research and aims to be at the forefront of the field. We welcome comprehensive articles, short communications, and review articles from established leaders in the rapidly evolving fields of materials science and related disciplines. We strive to provide authors with rigorous peer review, fast publication, and maximum exposure for their work. While we only accept the most significant manuscripts, our speedy evaluation process ensures that there are no unnecessary publication delays.
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