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Title

Effects of the Silicon Content on the Dimensional Changes of Electrodes for Lithium-ion Cells: An Electrochemical Dilatometry Study

Creator

Rodrigues Prado, Andressa Yasmim

Date

2021

Description

The continuous growth of the electric vehicle market has significantly increased the demand for Li-ion batteries (LIBs). However, state-of-the...
Show moreThe continuous growth of the electric vehicle market has significantly increased the demand for Li-ion batteries (LIBs). However, state-of-the-art LIBs are not yet able to meet the EV industry demand for high energy density and long cycle life rechargeable batteries, prompting efforts to improve the performance of Li-ion cells. In this context, silicon became the most promising next-generation active material for LIBs negative electrodes, especially because Si can significantly increase the lithium storage capacity of the commonly available anodes. Nonetheless, commercialization of Si-based electrodes has been hindered by the poor electrochemical performance of these electrodes, which is mainly attributed to the severe volumetric changes in the silicon particles related to the electrochemical reactions with Li. Since the electrodes are composites with a complex combination of various materials interspaced by pores, the electrode-level swelling may differ significantly from the particle-scale expansion. Furthermore, an increase in electrode thickness due to silicon expansion can have a direct effect on how Li-ion cells are designed, as the accommodation of electrode dilation requires additional cell space to prevent significant dynamic stresses. Thus, the actual volumetric energy density of a LIB cell depends on the electrode swelling, since the higher the magnitude of the electrode expansion, the lower the gains in energy density. Monitoring the electrode dilation is just as important as the electrochemical evaluation when designing cells with Si-based anodes.In this work, we use high-resolution operando electrochemical dilatometry to quantify the (de)lithiation-induced expansion/contraction of silicon, blended silicon-graphite and graphite electrodes, upon electrochemical cycling. We evaluate the relationship between electrode capacity and dilation and observe that while the lithiation capacity improved with increasing the silicon content, the electrode swelling is highly aggravated. For silicon-rich anodes, the electrode dilation can be higher than 300%, and the expansion profile consists of a combination of slow swelling at low levels of lithiation followed by an accelerated increase at higher lithium contents. This non-linear dilation allows for narrowing the swelling by limiting the electrode capacity. In addition, we investigate how electrode properties, such as porosity, affect the dilation profile, and quantify the irreversible expansion of the electrodes. Finally, we discuss some of the challenges associated with the dilatometry technique and suggest experimental approaches for obtaining consistent and reliable data.
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