Ni/Li Disordering in Layered Transition Metal Oxide: Electrochemical Impact, Origin, and Control.

Abstract:
Lithium ion batteries (LIBs) not only power most of today s hybrid electric vehicles (HEV) and electric vehicles (EV) but also are considered as a promising system for grid-level storage. Large-scale applications for LIBs require substantial improvement in energy density, cost, and lifetime. Layered lithium transition metal (TM) oxides, in particular, Li(Ni xMn yCo z)O2 (NMC, x + y + z = 1) are the most promising candidates as cathode materials with the potential to increase energy densities and lifetime, reduce costs, and improve safety. In order to further boost Li storage capacity, a great deal of attention has been directed toward developing Ni-rich layered TM oxides. However, structural disorder as a result of Ni/Li exchange in octahedral sites becomes a critical issue when Ni content increases to high values, as it leads to a detrimental effect on Li diffusivity, cycling stability, first-cycle efficiency, and overall electrode performance. Increasing effort has been dedicated to improving the electrochemical performance of layered TM oxides via reduction of cationic mixing. Therefore, it is important to summarize this research field and provide in-depth insight into the impact of Ni/Li disordering on electrochemical characteristics in layered TM oxides and its origin to accelerate the future development of layered TM oxides with high performance. In this Account, we start by introducing the Ni/Li disordering in LiNiO2, the experimental characterization of Ni/Li disordering, and analyzing the impact of Ni/Li disordering on electrochemical characteristics of layered TM oxides. The antisite Ni in the Li layer can limit the rate performance by impeding the Li ion transport. It will also degrade the cycling stability by inducing anisotropic stress in the bulk structure. Nevertheless, the antisite Ni ions do not always bring drawbacks to the electrochemical performance; some studies including our works found that it can improve the thermal stability and the cycling structure stability of Ni-rich NMC materials. We next discuss the driving forces and the kinetic advantages accounting for the Ni/Li exchange and conclude that the steric effect of cation size and the magnetic interactions between TM cations are the two main driving forces to promote the Ni/Li exchange during synthesis and the electrochemical cycling, and the low energy barrier of Ni2+ migration from the 3a site in the TM layer to the 3b site in the Li layer further provides a kinetic advantage. Based on this understanding, we then review the progress made to control the Ni/Li disordering through three main ways: (i) suppressing the driving force from the steric effect by ion exchange; (ii) tuning the magnetic interaction by cationic substitution; (iii) kinetically controlling Ni migration. Finally, our brief outlook on the future development of layered TM oxides with controlled Ni/Li disordering is provided. It is believed that this Account will provide significant understanding and inspirations toward developing high-performance layered TM oxide cathodes.
Author Listing： Jiaxin Zheng;Yaokun Ye;Tongchao Liu;Yinguo Xiao;Chongmin Wang;Feng Wang;Feng Pan
Volume： None
Pages： None
DOI： 10.1021/acs.accounts.9b00033
Language： English
Journal： Accounts of chemical research

ACCOUNTS OF CHEMICAL RESEARCH

Acc. Chem. Res.

影响因子：16.4 是否综述期刊：是 是否OA：否 是否预警：不在预警名单内 发行时间：1968 ISSN：0001-4842 发刊频率：Monthly 收录数据库：SCIE/Scopus收录 出版国家/地区：UNITED STATES 出版社：American Chemical Society

期刊介绍

Accounts of Chemical Research 主要发表化学和生物化学领域内关于基础研究和应用的短小精悍、具有作者团队自己研究特色的述评文章，或者前瞻性观点。这些短综述都是基于作者自己实验室的过往研究，以便向读者完整介绍研究项目。期刊收录研究方向：化学，化学综合Accounts of Chemical Research presents short, concise and critical articles offering easy-to-read overviews of basic research and applications in all areas of chemistry and biochemistry. These short reviews focus on research from the author’s own laboratory and are designed to teach the reader about a research project. In addition, Accounts of Chemical Research publishes commentaries that give an informed opinion on a current research problem. Special Issues online are devoted to a single topic of unusual activity and significance. Visit the Accounts Special Issues page for listings, descriptions, and TOC's of all special issues.Beginning in 2008, Accounts of Chemical Research replaced their traditional article abstract with an article "Conspectus." These new entries synopsize the research affording the reader a closer look at the content and significance of an article. Through this provision of a more detailed description of the article contents, the Conspectus enhances the article’s discoverability by search engines and the exposure for the research.

化学研究报告提供了简短，简洁和关键的文章，提供了化学和生物化学所有领域的基础研究和应用的易于阅读的概述。此外，《化学研究报告》还出版了专门针对异常活动和意义的单一问题的特刊。访问帐户特殊问题页面以获取所有特殊问题的列表，描述和目录。从2008年开始，化学研究帐户用文章 “Conspectus” 代替了传统的文章摘要。这些新条目概述了这项研究，使读者可以更仔细地了解文章的内容和意义。通过提供对文章内容的更详细描述，Conspectus增强了搜索引擎对文章的可发现性和对研究的了解。

年发文量 311
国人发稿量 102
国人发文占比 32.8%
自引率 0.6%
平均录取率 极难
平均审稿周期 一般,3-6周
版面费 -
偏重研究方向 化学-化学综合
期刊官网 https://pubs.acs.org/journal/achre4
投稿链接 https://acs.manuscriptcentral.com/acs

质量指标占比

研究类文章占比 OA被引用占比 撤稿占比 出版后修正文章占比
0.00% 12.32% 0.00% 0.90%

相关指数

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