In Situ Multilength-Scale Tracking of Dimensional and Viscoelastic Changes in Composite Battery Electrodes

Vadim Dargel, Nicolas Jäckel, Netanel Shpigel, Sergey Sigalov, Mikhael D. Levi, Leonid Daikhin, Volker Presser, Doron Aurbach

Research output: Contribution to journalArticlepeer-review

20 Scopus citations


Intercalation-induced dimensional changes in a composite battery electrode (comprising a polymeric binder) are one of the major factors limiting electrode cycling performance. Since electrode performance is expressed by the quantities averaged over its entire surface area (e.g., capacity retention, Faradaic efficiency, rate capability), significant efforts have been made to develop a methodology allowing its facile mechanical diagnostics at the same areal scale. Herein we introduce such a generic methodology for a highly sensitive in situ monitoring of intrinsic mechanical properties of composite battery electrodes. The gravimetric, dimensional, viscoelastic, and adhesive changes in the composite electrodes caused by Li-ions intercalation are assessed noninvasively and in real time by electrochemical quartz-crystal microbalance with dissipation monitoring (EQCM-D). Multiharmonic acoustic waves generated by EQCM-D penetrate into thin porous electrodes comprising either rigid or a soft binder resulting in frequency and dissipation changes quantified by analytical acoustic load impedance models. As a first demonstration, we used a composite LiFePO4 (LFP) electrode containing either polyvinylidene dichloride (PVdF) or Na carboximethyl cellulose (NaCMC) as rigid and viscoelastic binders, respectively, in aqueous electrolytes. The intercalation-induced volume changes of LFP electrode were evaluated from a hydrodynamic correction to the mass effect of the intercalated ions for PVdF, and both components of the effective complex shear modulus (i.e., storage and loss moduli) in case of NaCMC binder have been extracted. The sliding friction coefficients for large particles bound at their bottom to the quartz crystal surface (a measure of the adhesion strength of binders) has also been evaluated. Tracking the mechanical properties of the composite electrodes in different environments and charging/cycling conditions in a self-consistent manner provides all necessary conditions for an optimal selection of the polymeric binders resistant to intercalation-induced volume changes of intercalation particles.

Original languageEnglish
Pages (from-to)27664-27675
Number of pages12
JournalACS applied materials & interfaces
Issue number33
StatePublished - 23 Aug 2017

Bibliographical note

Publisher Copyright:
© 2017 American Chemical Society.


The authors acknowledge funding from the German-Israeli Foundation for Scientific Research and Development (GIF) via Research Grant Agreement No. 1-1237-302.5/2014. N.J. and V.P. thank Prof. Eduard Arzt (INM) for his continuing support.

FundersFunder number
German-Israeli Foundation for Scientific Research and Development
Research Grants Council, University Grants Committee1-1237-302.5/2014


    • EQCM
    • NaCMC
    • PVdF
    • QCM-D
    • composite electrodes
    • lithium ion battery
    • polymer binders


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