Investigating the impact of preparation routes on the properties of copper-decorated silicon particles as anode materials for lithium-ion batteries

Khryslyn G. Araño , Beth L. Armstrong , Anton W. Tomich , Matthew S. Chambers , Joseph Quinn , Harry M. Meyer III , Chanaka Kumara , Zoey Huey , Chun-Sheng Jiang , Chongmin Wang , Christopher S. Johnson , Raymond R. Unocic , Gabriel M. Veith
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Abstract

In recent years, the calendar life of Si has been recognized as a significant issue that must be addressed prior to technology deployment: The carbon conductive additive is a potential source of parasitic side reactions. However, carbon remains essential due to the low electronic conductivity of Si. In this study, we investigate the use of Cu as a conductive additive and potential alternative to carbon. Some Cu-decorated silicon particles (SiCu) were prepared using physical vapor deposition (PVD) via sputtering and high-energy milling. Other SiCu particles were prepared by using a solution method and examined briefly. The milling method caused Cu to appear as island-like features on the Si surface, whereas the PVD method initially produced similar island-like features that gradually developed into a continuous coating around the Si as sputtering time increased. Electrodes fabricated from SiCu exhibited lower overall resistivity, demonstrating the beneficial effect of Cu in improving electronic percolation through the electrode. Electrochemical tests showed that the milled SiCu exhibited higher capacity retention, improved rate capability, and lower overpotential. Furthermore, SiCu coupled with an NMC811 cathode exhibited lower leakage currents compared with the baseline silicon, indicating that incorporating Cu provided an additional advantage of minimizing parasitic currents in the cells.
研究了制备工艺对铜修饰硅颗粒作为锂离子电池负极材料性能的影响
近年来,硅的日历寿命已被认为是在技术部署之前必须解决的一个重要问题:碳导电添加剂是寄生副反应的潜在来源。然而,由于硅的低电子导电性,碳仍然是必不可少的。在这项研究中,我们研究了铜作为导电添加剂和潜在的碳替代品的使用。采用物理气相沉积(PVD)技术,通过溅射和高能铣削制备了一些cu修饰硅颗粒(SiCu)。采用溶液法制备了其他SiCu颗粒,并对其进行了简要的考察。铣削法使Cu在Si表面呈岛状特征,而PVD法最初产生类似的岛状特征,随着溅射时间的增加,逐渐发展成Si周围的连续涂层。用SiCu制备的电极显示出较低的总电阻率,证明了Cu在改善电子通过电极的渗透方面的有利作用。电化学测试结果表明,经磨后的SiCu具有较高的容量保留率、提高的速率性能和较低的过电位。此外,与基准硅相比,SiCu与NMC811阴极耦合显示出更低的泄漏电流,这表明结合Cu提供了最小化电池内寄生电流的额外优势。
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