Voltage hysteresis model for silicon electrodes for lithium ion batteries, including multi-step phase transformations, crystallization and amorphization
File(s)Jiang_2020_J._Electrochem._Soc._167_130533.pdf (1.48 MB)
Published version
Author(s)
Jiang, Yang
Offer, Gregory J
Jiang, Jun
Marinescu, Monica
Wang, Huizhi
Type
Journal Article
Abstract
Silicon has been an attractive alternative to graphite as an anode material in lithium-ion batteries (LIBs). The development of better silicon electrodes and the optimization of their operating conditions for longer cycle life require a quantitative understanding of the lithiation/delithiation mechanisms of silicon and how they are linked to the electrode behaviors. Herein we present a zero-dimensional mechanistic model of silicon anodes in LIBs. The model, for the first time, quantitatively accounts for the multi-step phase transformations, crystallization and amorphization of different lithium-silicon phases during cycling while being able to capture the electrode behaviors under different lithiation depths. Based on the model, a linkage between the underlying reaction processes and electrochemical performance is established. In particular, the two sloping voltage plateaus at low lithiation depth are correlated with two electrochemical phase transformations and the emergence of the single broad plateau at high lithiation depth is correlated with the amorphization of c-Li15Si4. The model is then used to study the effects of crystallization rate and surface energy barriers, which clarifies the role of surface energy and particle size in determining the performance behaviors of silicon. The model is a necessary tool for future design and development of high-energy-density, longer-life silicon-based LIBs.
Date Issued
2020-09-25
Date Acceptance
2020-09-25
Citation
Journal of the Electrochemical Society, 2020, 167 (13), pp.1-9
ISSN
0013-4651
Publisher
The Electrochemical Society
Start Page
1
End Page
9
Journal / Book Title
Journal of the Electrochemical Society
Volume
167
Issue
13
Copyright Statement
© 2020 The Author(s). This is an open access article distributed under the terms of the Creative Commons Attribution 4.0 License (CC BY, http://creativecommons.org/licenses/by/4.0/), which permits unrestricted reuse of the work in any medium, provided the original work is properly cited.
License URL
Identifier
https://iopscience.iop.org/article/10.1149/1945-7111/abbbba
Subjects
0303 Macromolecular and Materials Chemistry
0306 Physical Chemistry (incl. Structural)
0912 Materials Engineering
Energy
Publication Status
Published
Date Publish Online
2020-10-05