Design, Synthesis, and Characterization of a Novel Tetra-Block Copolymer for High-Performance Self-Healing Batteries.

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Title: Design, Synthesis, and Characterization of a Novel Tetra-Block Copolymer for High-Performance Self-Healing Batteries.
Authors: Avcı Yayla, Işık İpek1 (AUTHOR), Taskin, Omer Suat1,2 (AUTHOR), Yuca, Neslihan1,3 (AUTHOR)
Source: Polymers (20734360). Sep2025, Vol. 17 Issue 17, p2414. 15p.
Subjects: Lithium-ion batteries, Binding agents, Strains & stresses (Mechanics), Block copolymers, Electrochemical analysis, Silicon diodes, Energy storage
Abstract: Lithium-ion batteries (LIBs) have become the dominant energy storage technology due to their versatility and superior performance across diverse applications. Silicon (Si) stands out as a particularly promising high-capacity anode material for next-generation LIBs, offering a theoretical capacity nearly ten times greater than conventional graphite anodes. However, its practical implementation faces a critical challenge: the material undergoes a ~300% volume expansion during lithiation/delithiation, which causes severe mechanical stress, electrode pulverization, and rapid capacity decay. In addressing these limitations, advanced polymer binders serve as essential components for preserving the structural integrity of Si-based anodes. Notably, self-healing polymeric binders have emerged as a groundbreaking solution, capable of autonomously repairing cycle-induced damage and significantly enhancing electrode durability. The evaluation of self-healing performance is generally based on mechanical characterization methods while morphological observations by scanning electron microscopy provide direct evidence of crack closure; for electrochemically active materials, electrochemical techniques including GCD, EIS, and CV are employed to monitor recovery of functionality. In this study, a novel self-healing copolymer (PHX-23) was synthesized for Si anodes using a combination of octadecyl acrylate (ODA), methacrylic acid (MA), 2-hydroxyethyl methacrylate (HEMA), and polyethylene glycol methyl ether methacrylate (PEGMA). The copolymer was thoroughly characterized using NMR, FTIR, TGA, SEM, and EDX to confirm its chemical structure, thermal stability, and morphology. Electrochemical evaluation revealed that the PHX-23 binder markedly improves cycling stability, sustaining a reversible capacity of 427 mAh g−1 after 1000 cycles at 1C. During long-term cycling, the Coulombic efficiency of the PHX-23 polymer is 99.7%, and similar functional binders in the literature have shown similar results at lower C-rates. Comparative analysis with conventional binders (e.g., PVDF and CMC/SBR) demonstrated PHX-23's exceptional performance, exhibiting higher capacity retention and improved rate capability. These results position PHX-23 as a transformative binder for silicon anodes in next-generation lithium-ion batteries. [ABSTRACT FROM AUTHOR]
Copyright of Polymers (20734360) is the property of MDPI and its content may not be copied or emailed to multiple sites without the copyright holder's express written permission. Additionally, content may not be used with any artificial intelligence tools or machine learning technologies. However, users may print, download, or email articles for individual use. This abstract may be abridged. No warranty is given about the accuracy of the copy. Users should refer to the original published version of the material for the full abstract. (Copyright applies to all Abstracts.)
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  Data: Design, Synthesis, and Characterization of a Novel Tetra-Block Copolymer for High-Performance Self-Healing Batteries.
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  Data: <searchLink fieldCode="JN" term="%22Polymers+%2820734360%29%22">Polymers (20734360)</searchLink>. Sep2025, Vol. 17 Issue 17, p2414. 15p.
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  Data: <searchLink fieldCode="DE" term="%22Lithium-ion+batteries%22">Lithium-ion batteries</searchLink><br /><searchLink fieldCode="DE" term="%22Binding+agents%22">Binding agents</searchLink><br /><searchLink fieldCode="DE" term="%22Strains+%26+stresses+%28Mechanics%29%22">Strains & stresses (Mechanics)</searchLink><br /><searchLink fieldCode="DE" term="%22Block+copolymers%22">Block copolymers</searchLink><br /><searchLink fieldCode="DE" term="%22Electrochemical+analysis%22">Electrochemical analysis</searchLink><br /><searchLink fieldCode="DE" term="%22Silicon+diodes%22">Silicon diodes</searchLink><br /><searchLink fieldCode="DE" term="%22Energy+storage%22">Energy storage</searchLink>
– Name: Abstract
  Label: Abstract
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  Data: Lithium-ion batteries (LIBs) have become the dominant energy storage technology due to their versatility and superior performance across diverse applications. Silicon (Si) stands out as a particularly promising high-capacity anode material for next-generation LIBs, offering a theoretical capacity nearly ten times greater than conventional graphite anodes. However, its practical implementation faces a critical challenge: the material undergoes a ~300% volume expansion during lithiation/delithiation, which causes severe mechanical stress, electrode pulverization, and rapid capacity decay. In addressing these limitations, advanced polymer binders serve as essential components for preserving the structural integrity of Si-based anodes. Notably, self-healing polymeric binders have emerged as a groundbreaking solution, capable of autonomously repairing cycle-induced damage and significantly enhancing electrode durability. The evaluation of self-healing performance is generally based on mechanical characterization methods while morphological observations by scanning electron microscopy provide direct evidence of crack closure; for electrochemically active materials, electrochemical techniques including GCD, EIS, and CV are employed to monitor recovery of functionality. In this study, a novel self-healing copolymer (PHX-23) was synthesized for Si anodes using a combination of octadecyl acrylate (ODA), methacrylic acid (MA), 2-hydroxyethyl methacrylate (HEMA), and polyethylene glycol methyl ether methacrylate (PEGMA). The copolymer was thoroughly characterized using NMR, FTIR, TGA, SEM, and EDX to confirm its chemical structure, thermal stability, and morphology. Electrochemical evaluation revealed that the PHX-23 binder markedly improves cycling stability, sustaining a reversible capacity of 427 mAh g−1 after 1000 cycles at 1C. During long-term cycling, the Coulombic efficiency of the PHX-23 polymer is 99.7%, and similar functional binders in the literature have shown similar results at lower C-rates. Comparative analysis with conventional binders (e.g., PVDF and CMC/SBR) demonstrated PHX-23's exceptional performance, exhibiting higher capacity retention and improved rate capability. These results position PHX-23 as a transformative binder for silicon anodes in next-generation lithium-ion batteries. [ABSTRACT FROM AUTHOR]
– Name: AbstractSuppliedCopyright
  Label:
  Group: Ab
  Data: <i>Copyright of Polymers (20734360) is the property of MDPI and its content may not be copied or emailed to multiple sites without the copyright holder's express written permission. Additionally, content may not be used with any artificial intelligence tools or machine learning technologies. However, users may print, download, or email articles for individual use. This abstract may be abridged. No warranty is given about the accuracy of the copy. Users should refer to the original published version of the material for the full abstract.</i> (Copyright applies to all Abstracts.)
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      – Type: doi
        Value: 10.3390/polym17172414
    Languages:
      – Code: eng
        Text: English
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        PageCount: 15
        StartPage: 2414
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      – SubjectFull: Lithium-ion batteries
        Type: general
      – SubjectFull: Binding agents
        Type: general
      – SubjectFull: Strains & stresses (Mechanics)
        Type: general
      – SubjectFull: Block copolymers
        Type: general
      – SubjectFull: Electrochemical analysis
        Type: general
      – SubjectFull: Silicon diodes
        Type: general
      – SubjectFull: Energy storage
        Type: general
    Titles:
      – TitleFull: Design, Synthesis, and Characterization of a Novel Tetra-Block Copolymer for High-Performance Self-Healing Batteries.
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            NameFull: Avcı Yayla, Işık İpek
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            NameFull: Taskin, Omer Suat
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            NameFull: Yuca, Neslihan
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            – D: 01
              M: 09
              Text: Sep2025
              Type: published
              Y: 2025
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              Value: 17
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