A composite electrode model for lithium-ion batteries with silicon/graphite negative electrodes
File(s)Composite electrode modelling paper.pdf (1.7 MB)
Accepted version
Author(s)
Type
Journal Article
Abstract
Silicon is a promising negative electrode material with a high specific capacity, which is desirable for com-
mercial lithium-ion batteries. It is often blended with graphite to form a composite anode to extend lifetime,
however, the electrochemical interactions between silicon and graphite have not been fully investigated. Here,
an electrochemical composite electrode model is developed and validated for lithium-ion batteries with a
silicon/graphite anode. The continuum-level model can reproduce the voltage hysteresis and demonstrate
the interactions between graphite and silicon. At high states-of-charge, graphite provides the majority of the
reaction current density, however this rapidly switches to the silicon phase at deep depths-of-discharge due to
the different open circuit voltage curves, mass fractions and exchange current densities. Furthermore, operation
at high C-rates leads to heterogeneous current densities in the through-thickness direction, where peak reaction
current densities for silicon can be found at the current collector–electrode side as opposed to the separator–
electrode side for graphite. Increasing the mass fraction of silicon also highlights the beneficial impacts of
reducing the peak reaction current densities. This work, therefore, gives insights into the effects of silicon
additives, their coupled interactions and provides a platform to test different composite electrodes for better
lithium-ion batteries.
mercial lithium-ion batteries. It is often blended with graphite to form a composite anode to extend lifetime,
however, the electrochemical interactions between silicon and graphite have not been fully investigated. Here,
an electrochemical composite electrode model is developed and validated for lithium-ion batteries with a
silicon/graphite anode. The continuum-level model can reproduce the voltage hysteresis and demonstrate
the interactions between graphite and silicon. At high states-of-charge, graphite provides the majority of the
reaction current density, however this rapidly switches to the silicon phase at deep depths-of-discharge due to
the different open circuit voltage curves, mass fractions and exchange current densities. Furthermore, operation
at high C-rates leads to heterogeneous current densities in the through-thickness direction, where peak reaction
current densities for silicon can be found at the current collector–electrode side as opposed to the separator–
electrode side for graphite. Increasing the mass fraction of silicon also highlights the beneficial impacts of
reducing the peak reaction current densities. This work, therefore, gives insights into the effects of silicon
additives, their coupled interactions and provides a platform to test different composite electrodes for better
lithium-ion batteries.
Date Issued
2022-04
Date Acceptance
2022-02-05
Citation
Journal of Power Sources, 2022, 527, pp.231142-231142
ISSN
0378-7753
Publisher
Elsevier BV
Start Page
231142
End Page
231142
Journal / Book Title
Journal of Power Sources
Volume
527
Copyright Statement
© 2022 Elsevier B.V. All rights reserved
Sponsor
The Faraday Institution
Identifier
https://www.sciencedirect.com/science/article/pii/S0378775322001604?via%3Dihub
Grant Number
FIRG025
Subjects
03 Chemical Sciences
09 Engineering
Energy
Publication Status
Published
Article Number
231142
Date Publish Online
2022-02-24