Tuning the Morphology and Electronic Properties of Single-Crystal LiNi0.5Mn1.5O4−δ: Exploring the Influence of LiCl–KCl Molten Salt Flux Composition and Synthesis Temperature

熔盐 尖晶石 化学 电池(电) 阴极 焊剂(冶金) 电化学 相(物质) 相图 化学工程 同步加速器 Crystal(编程语言) 形态学(生物学) 分析化学(期刊) 无机化学 热力学 电极 材料科学 冶金 物理化学 功率(物理) 物理 有机化学 色谱法 核物理学 工程类 遗传学 生物 计算机科学 程序设计语言
作者
Stephanie Spence,Zhengrui Xu,Sami Sainio,Dennis Nordlund,Feng Lin
出处
期刊:Inorganic Chemistry [American Chemical Society]
卷期号:59 (15): 10591-10603 被引量:31
标识
DOI:10.1021/acs.inorgchem.0c01042
摘要

Single-crystal materials have played a unique role in the development of high-performance cathode materials for Li batteries due to their favorable chemomechanical stability. The molten salt synthesis method has become one of the most prominent techniques used to synthesize single-crystal layered and spinel materials. In this work, the molten salt synthesis method is used as a technique to tune both the morphology and Mn3+ content of high-voltage LiNi0.5Mn1.5O4 (LNMO) cathodes. The resulting materials are thoroughly characterized by a suite of analytical techniques, including synchrotron X-ray core-level spectroscopy, which are sensitive to the material properties on multiple length scales. The multidimensional characterization allows us to build a materials library according to the molten salt phase diagram as well as to establish the relationship among synthesis, material properties, and battery performance. The results of this work show that the Mn3+ content is primarily dependent on the synthesis temperature and increases as the temperature is increased. The particle morphology is mostly dependent on the composition of the molten salt flux, which can be tailored to obtain well-defined octahedrons enclosed by (111) facets, plates with predominant (112̅) facets, irregularly shaped particles, or mixtures of these. The electrochemical measurements indicate that the Mn3+ content has a larger contribution to the battery performance of LNMO than do morphological characteristics and that a significant amount of Mn3+ could become detrimental to the battery performance. However, with similar Mn3+ contents, morphology still plays a role in influencing the battery cycle life and rate performance. The insights of molten salt synthesis parameters on the formation of LNMO, with deconvolution of the roles of Mn3+ and morphology, are crucial to continuing studies in the rational design of LNMO cathode materials for high-energy Li batteries.
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