Characterization and Prediction of Polymer/Active Material Interface Failure in Battery Electrodes

Interface fracture is a critical issue for next-generation rechargeable batteries. The integrity of the binder/active material interface is essential for successful battery operation, and the interface failure is a major capacity fade mechanism. In spite of the importance, no systematic study on understanding/characterization of this issue exists at present. Here, the interface fracture was studied using a model polyvinylidene fluoride (PVdF)/Si system due to its importance in future Li-ion batteries. The interface failure was characterized in terms of critical energy release rate Gc using an experimental technique based on blister test and Michelson interferometry. The effect of the oxide layer on the interface fracture was also quantified. The critical energy release rate Gc of PVdF/Si interface is 0.55 ± 0.14 Jm−2, and the presence of oxide layer at the interface increased the Gc by an order of magnitude higher, i.e., the Gc of PVdF/SiO2 interface is 2.46 ± 0.40 Jm−2. The scanning electron microscopy (SEM) and X-ray photoelectron spectroscopy (XPS) analysis of the fracture surfaces showed that the crack growth mechanism is adhesive for both interface systems, and the strong adhesion of PVdF to SiO2 surface is attributed to the nature of bonding, i.e., a higher concentration of silanol (Si-OH) group on the SiO2 surface as compared to the Si surface to which PVdF forms a bond with. The experimental methodology proposed here is more general and can be used to study the fracture behavior of interfaces in other electrode systems and with other battery chemistries.

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Impact of Binder Thin-Films on Surface Chemistry of Silicon Anodes in Lithium-Ion Batteries

Johnson,

Waller,

Bezsonov

et al. 2024

ECS Adv.

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The effect of polymer binder on the nature and location of solid-electrolyte interphase (SEI) formation on Si active material was investigated. Thin layers of polymeric binder (polyvinylidene fluoride and sodium carboxymethyl cellulose) were spin-coated onto polished single crystal Si wafers. The samples were cycled against a Li counter/reference electrode under various electrochemical conditions in a coin cell configuration. The electrolyte was 1 M of LiPF6 in 1:1:1 wt % EC:DEC:DMC. After cycling, the samples were extracted from the coin cell under inert conditions and X-ray photoelectron spectroscopy (XPS) was performed. Electron microscopy and atomic force microscopy indicate that the binder films are smooth and continuous across the wafer surface, and no impact on the electrochemical behavior was observed. However, notable differences were detected using XPS, which revealed both difference in SEI composition and location relative to the binder-electrolyte and binder-substrate interfaces. These observations and insights will be useful in cell designs, binder selection, and reliability estimates because the location of SEI formation may influence cyclic performance of electrodes.

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Characterization and Prediction of Polymer/Active Material Interface Failure in Battery Electrodes

Cited by 3 publications

References 51 publications

Battery engineering safety technologies (BEST): M5 framework of mechanisms, modes, metrics, modeling, and mitigation

Battery engineering safety technologies (BEST): M5 framework of mechanisms, modes, metrics, modeling, and mitigation

Measurement of Binder/Active Material Interface Fracture in Rechargeable Batteries and the Effect of Oxide Coating

Impact of Binder Thin-Films on Surface Chemistry of Silicon Anodes in Lithium-Ion Batteries

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