插层(化学)
粒子(生态学)
锂(药物)
电解质
材料科学
电池(电)
相(物质)
化学物理
电极
无机化学
化学
热力学
物理
物理化学
地质学
内分泌学
功率(物理)
有机化学
海洋学
医学
作者
Aashutosh Mistry,Thomas M. M. Heenan,Kandler Smith,Paul R. Shearing,Partha P. Mukherjee
出处
期刊:ACS energy letters
[American Chemical Society]
日期:2022-05-05
卷期号:7 (5): 1871-1879
被引量:22
标识
DOI:10.1021/acsenergylett.2c00870
摘要
Uniform intercalation is desired to enable next-generation Li-ion batteries. While we expect nonuniformity in materials undergoing a phase change, single-phase intercalation materials such as nickel manganese cobalt oxide are believed to lithiate uniformly at the particle/electrolyte interface. However, recent imaging reveals nonuniform lithiation. Motivated by this discrepancy, we examine if aspherical particle shape can cause such nonuniformity since the conventional belief is based on spherical particle theory. We obtain real particle geometries using rapid lab-based X-ray computed tomography and subsequently perform physics-based calculations accounting for electrochemical reactions at the particle/electrolyte interface and lithium transport inside the particle bulk. The aspherical geometry breaks the symmetry and causes nonuniform reaction distribution. Such nonuniformity is exacerbated as the particle becomes more aspherical. The proposed mechanism represents a fundamental limit on achievable lithiation uniformity in aspherical particles in the absence of other mechanisms causing inhomogeneity, such as grain structure, nonuniform carbon-binder coating, etc.
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