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Restorable Neutralization of Poly(acrylic acid) Binders toward Balanced Processing Properties and Cycling Performance for Silicon Anodes in Lithium-Ion Batteries
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    Restorable Neutralization of Poly(acrylic acid) Binders toward Balanced Processing Properties and Cycling Performance for Silicon Anodes in Lithium-Ion Batteries
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    • Zhangxing Shi
      Zhangxing Shi
      Chemical Sciences and Engineering Division, Argonne National Laboratory, 9700 South Cass Avenue, Lemont, Illinois 60439, United States
    • Sisi Jiang
      Sisi Jiang
      Chemical Sciences and Engineering Division, Argonne National Laboratory, 9700 South Cass Avenue, Lemont, Illinois 60439, United States
      More by Sisi Jiang
    • Lily A. Robertson
      Lily A. Robertson
      Chemical Sciences and Engineering Division, Argonne National Laboratory, 9700 South Cass Avenue, Lemont, Illinois 60439, United States
      Joint Center for Energy Storage Research, 9700 South Cass Avenue, Lemont, Illinois 60439, United States
    • Yuyue Zhao
      Yuyue Zhao
      Chemical Sciences and Engineering Division, Argonne National Laboratory, 9700 South Cass Avenue, Lemont, Illinois 60439, United States
      Joint Center for Energy Storage Research, 9700 South Cass Avenue, Lemont, Illinois 60439, United States
      More by Yuyue Zhao
    • Erik Sarnello
      Erik Sarnello
      Department of Chemistry and Biochemistry, Northern Illinois University, DeKalb, Illinois 60115, United States
    • Tao Li
      Tao Li
      Department of Chemistry and Biochemistry, Northern Illinois University, DeKalb, Illinois 60115, United States
      X-ray Science Division, Advanced Photon Source, Argonne National Laboratory, Lemont, Illinois 60439, United States
      More by Tao Li
    • Wei Chen
      Wei Chen
      Institute for Molecular Engineering and Materials Science Division, Argonne National Laboratory, 9700 South Cass Avenue, Lemont, Illinois 60439, United States
      Institute for Molecular Engineering, The University of Chicago, 5640 South Ellis Avenue, Chicago, Illinois 60637, United States
      More by Wei Chen
    • Zhengcheng Zhang
      Zhengcheng Zhang
      Chemical Sciences and Engineering Division, Argonne National Laboratory, 9700 South Cass Avenue, Lemont, Illinois 60439, United States
      Joint Center for Energy Storage Research, 9700 South Cass Avenue, Lemont, Illinois 60439, United States
    • Lu Zhang*
      Lu Zhang
      Chemical Sciences and Engineering Division, Argonne National Laboratory, 9700 South Cass Avenue, Lemont, Illinois 60439, United States
      Joint Center for Energy Storage Research, 9700 South Cass Avenue, Lemont, Illinois 60439, United States
      *Email: [email protected]
      More by Lu Zhang
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    ACS Applied Materials & Interfaces

    Cite this: ACS Appl. Mater. Interfaces 2020, 12, 52, 57932–57940
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acsami.0c18559
    Published December 16, 2020
    Copyright © 2020 American Chemical Society

    Abstract

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    Neutralization of poly(acrylic acid) (PAA)-based binders using lithium hydroxide is a common strategy for fabricating silicon anode laminates, which improves rheological properties of slurries toward high-quality electrode laminates. However, the significantly increased basicity causes degradation of Si particles while the irreversible conversion of carboxylic acid groups to lithium carboxylates undermines the binding strength, collectively leading to adverse cycling performance of the fabricated Si anodes. Herein, a novel neutralization process for PAA binders is developed. A weak base, ammonia (NH3), was discovered as a neutralizing agent that still promotes rheological response of binder solutions but results in a reduced pH increase. Interestingly, the resulting ammonium carboxylate groups may cleave during the drying process to restore the neutralized PAA (PAA-NH3) binders to their pristine states. The best-performing composition of 50% neutralization (PAA-50%NH3) provides comparable rheological response as a PAA-Li binder as well as much improved cycling performance. The half-cells using the PAA-50%NH3 binder can deliver 60% capacity retention over 100 cycles at C/3 rate, affording a 23.8% increase compared to PAA-Li half-cells. This restorable neutralization process of PAA binders represents an innovative strategy of mitigating issues from slurry processing of Si particles to achieve concurrent improvements in high-quality lamination and cycling performance.

    Copyright © 2020 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.0c18559.

    • The pH values of binder solutions, FTIR, SEM images, SAXS profiles, details regarding full cell cycling, and images of slurries (PDF)

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    This article is cited by 25 publications.

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    ACS Applied Materials & Interfaces

    Cite this: ACS Appl. Mater. Interfaces 2020, 12, 52, 57932–57940
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acsami.0c18559
    Published December 16, 2020
    Copyright © 2020 American Chemical Society

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