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Investigations on the effect of current density on SiO/Si composite electrodes

By Xiong, Jie; Yang, Jian; Wang, Guanyi; Saeed, Tahseen; Liu, Yuzi; Kaczmarek, Stephen E.; Lu, Wenquan; Wu, Qingliu
Published in Electrochimica Acta 2021

Abstract

An oxide layer on the surface of silicon particles is inevitable and is necessary for their application as anode materials for lithium ion batteries with high capacity and durability. However, a thick surficial oxide layer could significantly reduce the capacity of a Si anode. In this study, Si nanoparticles with a thick surficial oxide layer of ∼20 nm (Si@SiOx) were fabricated through thermal oxidation and investigated electrochemically. The results revealed that very low current density is needed to activate Si@SiOx anodes during the first formation cycle. Once activated, the Si@SiOx anode can deliver reversible capacity as high as ∼1000 mAh/g with low current density. Then, the Si@SiOx can be cycled at higher current densities of >700 mAh/g. Electrochemical impedance spectroscopy (EIS) shows that the lower current density results in lower charge-transfer resistance of the Si@SiOx anode, suggesting a higher degree of lithiation of the surficial oxide layer during low-current activation. EIS analysis also reveals that the lithiation of the surficial oxide is irreversible. We believe that the surface silicon oxide layer is lithiated and forms lithium silicate during the initial activation process. Lithium silicate has high conductivity and allows the lithiation/delithiation of Si core under the oxide layer during following charge and discharge.

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