Spherical Graphite Anodes: Influence of Particle Size Distribution and Multilayer Structuring in Lithium-Ion Battery Cells

Laura Gottschalk, Jannes Müller, Alexander Schoo, Ernesto Baasch, Arno Kwade
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Abstract

Current research focuses on lithium-ion battery cells with a high energy density and efficient fast-charging capabilities. However, transport limitations, and, therefore, the uniform diffusion of lithium-ions across the electrode layers, remain a challenge and could lead to reduced cell performance. One approach to overcome these transport challenges is the use of subsequently produced two-layer anodes with the particle size variation of spherical graphite (x50 = 18 µm; x50 = 11 µm). Thereby, a defined pore network is created, which reduces the ionic resistance and ensuring improved fast charging capabilities. The analysis focuses on the evaluation of electrode properties and the electrochemical performance. By examining the pore size distribution of the anodes, it has been found that during the manufacturing of the two-layer anodes, carbon black and binder particles are transported into the existing microstructure of the lower layer, resulting in localized densification between the anode layers. This could also be supported by color measurements. This effect also extends to electrochemical investigations, with electrochemical impedance spectroscopy showing significantly lower ionic resistances in all two-layer anodes. Reduced ionic resistance and tortuosity near the separator due to absorption effects enhance the ion diffusion and have a direct impact on anode performance. Cell ageing analysis showed a significant capacity decrease of almost 15 mAh g −1 in the single-layer references only, in contrast to the stability of the two-layer anodes. This could also be attributed to the reduced ionic resistance and active counteraction of binder migration. In conclusion, this study highlights how subsequently produced two-layer anodes significantly shape the electrode properties and cell performance of lithium-ion batteries.
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球形石墨阳极:锂离子电池中颗粒尺寸分布和多层结构的影响
目前的研究重点是具有高能量密度和高效快速充电能力的锂离子电池。然而,传输限制以及锂离子在电极层间的均匀扩散仍然是一个挑战,并可能导致电池性能下降。克服这些传输难题的一种方法是使用随后生产的具有球形石墨粒度变化(x50 = 18 µm;x50 = 11 µm)的双层阳极。这样就形成了一个确定的孔隙网络,从而降低了离子阻力,确保提高快速充电能力。分析的重点是评估电极特性和电化学性能。通过研究阳极的孔径分布,发现在制造双层阳极的过程中,炭黑和粘合剂颗粒被输送到下层现有的微观结构中,导致阳极层之间局部致密化。颜色测量结果也证明了这一点。这种效应还延伸到电化学研究中,电化学阻抗谱显示所有双层阳极的离子电阻都显著降低。由于吸收效应,分离器附近的离子电阻和迂回度降低,从而增强了离子扩散,并对阳极性能产生了直接影响。电池老化分析表明,与双层阳极的稳定性相比,只有单层阳极的容量显著下降了近 15 mAh g -1 。这也可能归因于离子电阻的降低和粘结剂迁移的积极反作用。总之,本研究强调了后续生产的双层阳极如何显著影响锂离子电池的电极特性和电池性能。
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