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

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    Energy, Environmental, and Catalysis Applications

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

    Cite this: ACS Appl. Mater. Interfaces 2022, 14, 20, 23322–23331
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    https://doi.org/10.1021/acsami.2c00723
    Published May 16, 2022
    Copyright © 2022 The Authors. Published by American Chemical Society
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    Abstract

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    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.

    Copyright © 2022 The Authors. Published by American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsami.2c00723.

    • SEM/EDX, refractive index, USANS, and SANS figures along with tables summarizing the fits to the USANS and SANS data are presented in the Supplemental Information Section (PDF)

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    Cited By

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    This article is cited by 5 publications.

    1. James Parker, Rachel Smith, Denis Cumming. High-Resolution X-ray Mapping of Fluorinated Binders in Lithium-Ion Battery Electrodes. The Journal of Physical Chemistry C 2024, Article ASAP.
    2. Jonas Grill, Jelena Popovic-Neuber. Cation Conducting Binders: From Liquid to Solid-State Batteries. ACS Energy Letters 2024, 9 (9) , 4465-4474. https://doi.org/10.1021/acsenergylett.4c01684
    3. Zhaomei Sun, Jiadeng Zhu, Chen Yang, Qibao Xie, Yan Jiang, Kaixiang Wang, Mengjin Jiang. N-Type Polyoxadiazole Conductive Polymer Binders Derived High-Performance Silicon Anodes Enabled by Crosslinking Metal Cations. ACS Applied Materials & Interfaces 2023, 15 (10) , 12946-12956. https://doi.org/10.1021/acsami.2c19587
    4. Changkai Zhao, Anuj Kumar, Zongge Li, Luman He, Xiangshe Meng, Nianxi Liu, Mei Guo, Zhiming Liu, Gang Dou, Yaqun Wang, Guoxin Zhang. N4-Vacancy-Functionalized Carbon for High-Rate Li-Ion Storage. ACS Applied Materials & Interfaces 2022, 14 (45) , 50794-50802. https://doi.org/10.1021/acsami.2c13425
    5. Wenqiang Zhu, Jun Zhou, Fan Zhang, Tingting Li, Yahui Yang, Jiang Yin, Zhongliang Tian, Wenzhang Li, Yanqing Lai, Lishan Yang. Sustainable silicon micro-dendritic anodes integrated by a moderately cross-linked polymer binder with superior elasticity and adhesion. Journal of Alloys and Compounds 2022, 926 , 166858. https://doi.org/10.1016/j.jallcom.2022.166858
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    ACS Applied Materials & Interfaces

    Cite this: ACS Appl. Mater. Interfaces 2022, 14, 20, 23322–23331
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acsami.2c00723
    Published May 16, 2022
    Copyright © 2022 The Authors. Published by American Chemical Society
    Request reuse permissions

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