Understanding the Solution Dynamics and Binding of a PVDF Binder with Silicon, Graphite, and NMC Materials and the Influence on Cycling Performance

Mary K. Burdette-Trofimov; Beth L. Armstrong; Rachel J. Korkosz; J. Landon Tyler; Rebecca D. McAuliffe; Luke Heroux; Mathieu Doucet; David T. Hoelzer; Nihal Kanbargi; Amit K. Naskar; Gabriel M. Veith

doi:10.1021/acsami.2c00723

Understanding the Solution Dynamics and Binding of a PVDF Binder with Silicon, Graphite, and NMC Materials and the Influence on Cycling Performance

Mary K. Burdette-Trofimov, Beth L. Armstrong, Rachel J. Korkosz, J. Landon Tyler, Rebecca D. McAuliffe, Luke Heroux, Mathieu Doucet, David T. Hoelzer, Nihal Kanbargi, Amit K. Naskar, Gabriel M. Veith

Research output: Contribution to journal › Article › peer-review

9 Scopus citations

Abstract

The impact of the binding, solution structure, and solution dynamics of poly(vinylidene fluoride) (PVDF) with silicon on its performance as compared to traditional graphite and Li_1.05Ni_0.33Mn_0.33Co_0.33O₂(NMC) electrode materials was explored. Through refractive index (RI) measurements, the concentration of the binder adsorbed on the surface of electrode materials during electrode processing was determined to be less than half of the potentially available material resulting in excessive free binder in solution. Using ultrasmall-angle neutron scattering (USANS) and small-angle neutron scattering (SANS), it was found that PVDF forms a conformal coating over the entirety of the silicon particle. This is in direct contrast to graphite-PVDF and NMC-PVDF slurries, where PVDF only covers part of the graphite surface, and the PVDF chains make a network-like graphite-PVDF structure. Conversely, a thick layer of PVDF covers NMC particles, but the coating is porous, allowing for ion and electronic transport. The homogeneous coating of silicon breaks up percolation pathways, resulting in poor cycling performance of silicon materials as widely reported. These results indicate that the Si-PVDF interactions could be modified from a binder to a dispersant.

Original language	English
Pages (from-to)	23322-23331
Number of pages	10
Journal	ACS Applied Materials and Interfaces
Volume	14
Issue number	20
DOIs	https://doi.org/10.1021/acsami.2c00723
State	Published - May 25 2022

Funding

The authors would like to thank Tim Armstrong of Steward Advanced Materials for the commercial sample of the NMC. This research (M.K.B.-T., B.L.A., R.J.K., J.L.T., R.D.M., D.T.H., and G.M.V.) was supported by the US Department of Energy’s Vehicle Technologies Office under the Silicon Consortium Project, directed by Brian Cunningham, and managed by Anthony Burrell. A portion of this research used resources at the Spallation Neutron Source, a DOE Office of Science User Facility operated by Oak Ridge National Laboratory (M.D. and L.H.). The small-angle scattering measurements were done using the USANS and EQSANS instruments at the Spallation Neutron Source. This work benefited from the use of the SasView application, originally developed under NSF award DMR-0520547. SasView contains code developed with funding from the European Union’s Horizon 2020 research and innovation program under the SINE2020 project, grant agreement no. 654000. The authors thank Paul Dodson and Bill Aronoff for their invaluable help with the GPC. N.K. and A.K.N. thank Sumit Gupta and Siddhant Datta for assistance with EDXS measurements. This manuscript has been authored by UT-Battelle, LLC, under Contract DE-AC05-00OR22725 with the US Department of Energy. The United States Government retains and the publisher, by accepting the article for publication, acknowledges that the United States Government retains a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript, or allow others to do so, for United States Government purposes. The Department of Energy will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan ( http://energy.gov/downloads/doe-public-access-plan ).

Funders	Funder number
National Science Foundation	DMR-0520547
U.S. Department of Energy
Horizon 2020 Framework Programme	DE-AC05-00OR22725, 654000

Keywords

PVDF
battery electrode
binder
electrode processing
silicon anode

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

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10.1021/acsami.2c00723

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Burdette-Trofimov, M. K., Armstrong, B. L., Korkosz, R. J., Tyler, J. L., McAuliffe, R. D., Heroux, L., Doucet, M., Hoelzer, D. T., Kanbargi, N., Naskar, A. K., & Veith, G. M. (2022). Understanding the Solution Dynamics and Binding of a PVDF Binder with Silicon, Graphite, and NMC Materials and the Influence on Cycling Performance. ACS Applied Materials and Interfaces, 14(20), 23322-23331. https://doi.org/10.1021/acsami.2c00723

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title = "Understanding the Solution Dynamics and Binding of a PVDF Binder with Silicon, Graphite, and NMC Materials and the Influence on Cycling Performance",

abstract = "The impact of the binding, solution structure, and solution dynamics of poly(vinylidene fluoride) (PVDF) with silicon on its performance as compared to traditional graphite and Li1.05Ni0.33Mn0.33Co0.33O2(NMC) electrode materials was explored. Through refractive index (RI) measurements, the concentration of the binder adsorbed on the surface of electrode materials during electrode processing was determined to be less than half of the potentially available material resulting in excessive free binder in solution. Using ultrasmall-angle neutron scattering (USANS) and small-angle neutron scattering (SANS), it was found that PVDF forms a conformal coating over the entirety of the silicon particle. This is in direct contrast to graphite-PVDF and NMC-PVDF slurries, where PVDF only covers part of the graphite surface, and the PVDF chains make a network-like graphite-PVDF structure. Conversely, a thick layer of PVDF covers NMC particles, but the coating is porous, allowing for ion and electronic transport. The homogeneous coating of silicon breaks up percolation pathways, resulting in poor cycling performance of silicon materials as widely reported. These results indicate that the Si-PVDF interactions could be modified from a binder to a dispersant.",

keywords = "PVDF, battery electrode, binder, electrode processing, silicon anode",

author = "Burdette-Trofimov, {Mary K.} and Armstrong, {Beth L.} and Korkosz, {Rachel J.} and Tyler, {J. Landon} and McAuliffe, {Rebecca D.} and Luke Heroux and Mathieu Doucet and Hoelzer, {David T.} and Nihal Kanbargi and Naskar, {Amit K.} and Veith, {Gabriel M.}",

year = "2022",

month = may,

day = "25",

doi = "10.1021/acsami.2c00723",

language = "English",

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Burdette-Trofimov, MK, Armstrong, BL, Korkosz, RJ, Tyler, JL, McAuliffe, RD, Heroux, L , Doucet, M , Hoelzer, DT , Kanbargi, N , Naskar, AK & Veith, GM 2022, 'Understanding the Solution Dynamics and Binding of a PVDF Binder with Silicon, Graphite, and NMC Materials and the Influence on Cycling Performance', ACS Applied Materials and Interfaces, vol. 14, no. 20, pp. 23322-23331. https://doi.org/10.1021/acsami.2c00723

Understanding the Solution Dynamics and Binding of a PVDF Binder with Silicon, Graphite, and NMC Materials and the Influence on Cycling Performance. / Burdette-Trofimov, Mary K.; Armstrong, Beth L.; Korkosz, Rachel J. et al.
In: ACS Applied Materials and Interfaces, Vol. 14, No. 20, 25.05.2022, p. 23322-23331.

Research output: Contribution to journal › Article › peer-review

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T1 - Understanding the Solution Dynamics and Binding of a PVDF Binder with Silicon, Graphite, and NMC Materials and the Influence on Cycling Performance

AU - Burdette-Trofimov, Mary K.

AU - Armstrong, Beth L.

AU - Korkosz, Rachel J.

AU - Tyler, J. Landon

AU - McAuliffe, Rebecca D.

AU - Heroux, Luke

AU - Doucet, Mathieu

AU - Hoelzer, David T.

AU - Kanbargi, Nihal

AU - Naskar, Amit K.

AU - Veith, Gabriel M.

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N2 - The impact of the binding, solution structure, and solution dynamics of poly(vinylidene fluoride) (PVDF) with silicon on its performance as compared to traditional graphite and Li1.05Ni0.33Mn0.33Co0.33O2(NMC) electrode materials was explored. Through refractive index (RI) measurements, the concentration of the binder adsorbed on the surface of electrode materials during electrode processing was determined to be less than half of the potentially available material resulting in excessive free binder in solution. Using ultrasmall-angle neutron scattering (USANS) and small-angle neutron scattering (SANS), it was found that PVDF forms a conformal coating over the entirety of the silicon particle. This is in direct contrast to graphite-PVDF and NMC-PVDF slurries, where PVDF only covers part of the graphite surface, and the PVDF chains make a network-like graphite-PVDF structure. Conversely, a thick layer of PVDF covers NMC particles, but the coating is porous, allowing for ion and electronic transport. The homogeneous coating of silicon breaks up percolation pathways, resulting in poor cycling performance of silicon materials as widely reported. These results indicate that the Si-PVDF interactions could be modified from a binder to a dispersant.

AB - The impact of the binding, solution structure, and solution dynamics of poly(vinylidene fluoride) (PVDF) with silicon on its performance as compared to traditional graphite and Li1.05Ni0.33Mn0.33Co0.33O2(NMC) electrode materials was explored. Through refractive index (RI) measurements, the concentration of the binder adsorbed on the surface of electrode materials during electrode processing was determined to be less than half of the potentially available material resulting in excessive free binder in solution. Using ultrasmall-angle neutron scattering (USANS) and small-angle neutron scattering (SANS), it was found that PVDF forms a conformal coating over the entirety of the silicon particle. This is in direct contrast to graphite-PVDF and NMC-PVDF slurries, where PVDF only covers part of the graphite surface, and the PVDF chains make a network-like graphite-PVDF structure. Conversely, a thick layer of PVDF covers NMC particles, but the coating is porous, allowing for ion and electronic transport. The homogeneous coating of silicon breaks up percolation pathways, resulting in poor cycling performance of silicon materials as widely reported. These results indicate that the Si-PVDF interactions could be modified from a binder to a dispersant.

KW - PVDF

KW - battery electrode

KW - binder

KW - electrode processing

KW - silicon anode

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DO - 10.1021/acsami.2c00723

M3 - Article

AN - SCOPUS:85131126067

SN - 1944-8244

VL - 14

SP - 23322

EP - 23331

JO - ACS Applied Materials and Interfaces

JF - ACS Applied Materials and Interfaces

IS - 20

ER -

Understanding the Solution Dynamics and Binding of a PVDF Binder with Silicon, Graphite, and NMC Materials and the Influence on Cycling Performance

Abstract

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Keywords

UN SDGs

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