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Semi-rigid methyl substitution strategy for decoupling conflicting properties in transparent and thermally robust polyimide.

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Title: Semi-rigid methyl substitution strategy for decoupling conflicting properties in transparent and thermally robust polyimide.
Authors: Xu, Zhenqi1 (AUTHOR), Zhao, Rui2 (AUTHOR), Lu, Zhen1 (AUTHOR) Luzhen94@fzu.edu.cn, Hou, Linxi1,2,3,4 (AUTHOR) lxhou@fzu.edu.cn
Source: Journal of Polymer Research. May2026, Vol. 33 Issue 5, p1-13. 13p.
Subjects: Polyimides, Methyl groups, Thermal stability, Thermal expansion, Transparency (Optics), Copolymerization, Density functional theory, Mechanical behavior of materials
Abstract: Polyimide (PI) constitutes an indispensable class of materials for advanced optoelectronic devices. However, the simultaneous realization of high optical transparency, superior thermal stability, and thermoplastic processability remains a formidable challenge owing to intrinsic conflicts in conventional molecular design. To decouple these competing attributes, a semi-rigid methyl substitution strategy is introduced. A series of plasticized colorless polyimides (PCPI) is synthesized via copolymerization of 4,4'-(Hexafluoroisopropylidene) diphthalic anhydride (6FDA) and 4,4'-oxydianiline (ODA) with two methyl-substituted diamines. As methyl unit content increases, optical transmittance rises, with the optimal composition (semi-rigid unit/6FDA = 1:1) achieving an average transparency (Tavg) of 90% along with excellent solubility. All PCPIs maintain high thermal stability, exhibiting decomposition temperatures (the 10% weight temperature, Td10) exceeding 530 °C, a low coefficient of thermal expansion (CTE), and glass transition temperatures (Tg) around 300 °C. The toughness of these PI films was further supported by their high tensile strength. Theoretical modeling and Density Functional Theory (DFT) calculations reveal that the methyl groups and the semi-rigid backbone collectively balance chain packing and charge transfer interactions, leading to synergistic property enhancement. This work offers a practical and effective structural design route to high-performance PCPIs through controlled rigidity modulation. [ABSTRACT FROM AUTHOR]
Copyright of Journal of Polymer Research is the property of Springer Nature 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: Semi-rigid methyl substitution strategy for decoupling conflicting properties in transparent and thermally robust polyimide.
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  Data: <searchLink fieldCode="DE" term="%22Polyimides%22">Polyimides</searchLink><br /><searchLink fieldCode="DE" term="%22Methyl+groups%22">Methyl groups</searchLink><br /><searchLink fieldCode="DE" term="%22Thermal+stability%22">Thermal stability</searchLink><br /><searchLink fieldCode="DE" term="%22Thermal+expansion%22">Thermal expansion</searchLink><br /><searchLink fieldCode="DE" term="%22Transparency+%28Optics%29%22">Transparency (Optics)</searchLink><br /><searchLink fieldCode="DE" term="%22Copolymerization%22">Copolymerization</searchLink><br /><searchLink fieldCode="DE" term="%22Density+functional+theory%22">Density functional theory</searchLink><br /><searchLink fieldCode="DE" term="%22Mechanical+behavior+of+materials%22">Mechanical behavior of materials</searchLink>
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  Data: Polyimide (PI) constitutes an indispensable class of materials for advanced optoelectronic devices. However, the simultaneous realization of high optical transparency, superior thermal stability, and thermoplastic processability remains a formidable challenge owing to intrinsic conflicts in conventional molecular design. To decouple these competing attributes, a semi-rigid methyl substitution strategy is introduced. A series of plasticized colorless polyimides (PCPI) is synthesized via copolymerization of 4,4'-(Hexafluoroisopropylidene) diphthalic anhydride (6FDA) and 4,4'-oxydianiline (ODA) with two methyl-substituted diamines. As methyl unit content increases, optical transmittance rises, with the optimal composition (semi-rigid unit/6FDA = 1:1) achieving an average transparency (Tavg) of 90% along with excellent solubility. All PCPIs maintain high thermal stability, exhibiting decomposition temperatures (the 10% weight temperature, Td10) exceeding 530 °C, a low coefficient of thermal expansion (CTE), and glass transition temperatures (Tg) around 300 °C. The toughness of these PI films was further supported by their high tensile strength. Theoretical modeling and Density Functional Theory (DFT) calculations reveal that the methyl groups and the semi-rigid backbone collectively balance chain packing and charge transfer interactions, leading to synergistic property enhancement. This work offers a practical and effective structural design route to high-performance PCPIs through controlled rigidity modulation. [ABSTRACT FROM AUTHOR]
– Name: AbstractSuppliedCopyright
  Label:
  Group: Ab
  Data: <i>Copyright of Journal of Polymer Research is the property of Springer Nature 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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RecordInfo BibRecord:
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        Value: 10.1007/s10965-026-04938-y
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      – Code: eng
        Text: English
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        PageCount: 13
        StartPage: 1
    Subjects:
      – SubjectFull: Polyimides
        Type: general
      – SubjectFull: Methyl groups
        Type: general
      – SubjectFull: Thermal stability
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      – SubjectFull: Thermal expansion
        Type: general
      – SubjectFull: Transparency (Optics)
        Type: general
      – SubjectFull: Copolymerization
        Type: general
      – SubjectFull: Density functional theory
        Type: general
      – SubjectFull: Mechanical behavior of materials
        Type: general
    Titles:
      – TitleFull: Semi-rigid methyl substitution strategy for decoupling conflicting properties in transparent and thermally robust polyimide.
        Type: main
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          Name:
            NameFull: Xu, Zhenqi
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            NameFull: Zhao, Rui
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            NameFull: Lu, Zhen
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            NameFull: Hou, Linxi
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            – D: 01
              M: 05
              Text: May2026
              Type: published
              Y: 2026
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              Value: 33
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            – TitleFull: Journal of Polymer Research
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