3D Quantification of Elemental Gradients within Heterostructured Particles of Battery Cathodes
3D Quantification of Elemental Gradients within Heterostructured Particles of Battery Cathodes
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DOI：
10.1021/acsenergylett.2c02619
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发表时间：
2023-02
影响因子：
22
通讯作者：
E. Allen;Young-Seop Shin;William Judge;M. Wolfman;V. De Andrade;S. Cologna;J. Cabana
中科院分区：
文献类型：
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作者：
E. Allen;Young-Seop Shin;William Judge;M. Wolfman;V. De Andrade;S. Cologna;J. Cabana
已经追求具有在颗粒内定制的元素梯度的异质结构以对抗限制用于锂离子电池的富Ni阴极材料的不稳定性。不同组成层的生长在氢氧化物前体的合成过程中完成。然而，这些浓度梯度在高温反应期间被改变的程度难以以其完整的球形形式建立。在这里，我们展示了整个三维结构的二次粒子可以解决非破坏性的差分X射线吸收光谱（XAS）通过透射X射线显微镜（TXM）。颗粒位置和元素含量之间的关系被充分量化，具有高的统计意义，异质结构具有不同的组成梯度的前体与90：5：5 Ni：Mn：Co核心组成。高温合成后观察到元素异质性降低，但梯度仍然存在。所提出的方法应用于指导合成，同时确保电化学性能的增益与纳米级的精确元素分布有关。
Heterogenous architectures with elemental gradients tailored within particles have been pursued to combat the instabilities limiting Ni-rich cathode materials for lithium-ion batteries. The growth of different compositional layers is accomplished during the synthesis of hydroxide precursors. However, the extent to which these concentration gradients are modified during high-temperature reactions is difficult to establish in their intact, spherical form. Here, we show the entire three-dimensional structure of a secondary particle can be resolved nondestructively with differential X-ray absorption spectroscopy (XAS) through transmission X-ray microscopy (TXM). The relationship between particle location and elemental content was fully quantified, with high statistical significance, for heterostructures possessing different compositional gradients in the precursors with 90:5:5 Ni:Mn:Co core compositions. Reduced elemental heterogeneity was observed after high-temperature synthesis, but gradients remained. The methodology presented should be used to guide synthesis while assuring that gains in electrochemical performance are linked to precise elemental distributions at the nanoscale.