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Mechanochemically accessing a challenging-to-synthesize depolymerizable polymer

Author

Listed:
  • Tze-Gang Hsu

    (The University of Akron)

  • Shiqi Liu

    (The University of Akron)

  • Xin Guan

    (The University of Akron)

  • Seiyoung Yoon

    (The University of Akron)

  • Junfeng Zhou

    (The University of Akron)

  • Wei-Yuan Chen

    (The University of Akron)

  • Sanjay Gaire

    (The University of Akron)

  • Joshua Seylar

    (The University of Akron)

  • Hanlin Chen

    (The University of Akron)

  • Zeyu Wang

    (The University of Akron)

  • Jared Rivera

    (The University of Akron)

  • Leyao Wu

    (The University of Akron)

  • Christopher J. Ziegler

    (The University of Akron)

  • Ruel McKenzie

    (The University of Akron)

  • Junpeng Wang

    (The University of Akron)

Abstract

Polymers with low ceiling temperatures (Tc) are highly desirable as they can depolymerize under mild conditions, but they typically suffer from demanding synthetic conditions and poor stability. We envision that this challenge can be addressed by developing high-Tc polymers that can be converted into low-Tc polymers on demand. Here, we demonstrate the mechanochemical generation of a low-Tc polymer, poly(2,5-dihydrofuran) (PDHF), from an unsaturated polyether that contains cyclobutane-fused THF in each repeat unit. Upon mechanically induced cycloreversion of cyclobutane, each repeat unit generates three repeat units of PDHF. The resulting PDHF completely depolymerizes into 2,5-dihydrofuran in the presence of a ruthenium catalyst. The mechanochemical generation of the otherwise difficult-to-synthesize PDHF highlights the power of polymer mechanochemistry in accessing elusive structures. The concept of mechanochemically regulating the Tc of polymers can be applied to develop next-generation sustainable plastics.

Suggested Citation

  • Tze-Gang Hsu & Shiqi Liu & Xin Guan & Seiyoung Yoon & Junfeng Zhou & Wei-Yuan Chen & Sanjay Gaire & Joshua Seylar & Hanlin Chen & Zeyu Wang & Jared Rivera & Leyao Wu & Christopher J. Ziegler & Ruel Mc, 2023. "Mechanochemically accessing a challenging-to-synthesize depolymerizable polymer," Nature Communications, Nature, vol. 14(1), pages 1-9, December.
    • Handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-35925-2
    DOI: 10.1038/s41467-023-35925-2
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    References listed on IDEAS

    as
    1. Junpeng Wang & Tatiana B. Kouznetsova & Roman Boulatov & Stephen L. Craig, 2016. "Mechanical gating of a mechanochemical reaction cascade," Nature Communications, Nature, vol. 7(1), pages 1-8, December.
    2. Huan Zhang & Xun Li & Yangju Lin & Fei Gao & Zhen Tang & Peifeng Su & Wenke Zhang & Yuanze Xu & Wengui Weng & Roman Boulatov, 2017. "Multi-modal mechanophores based on cinnamate dimers," Nature Communications, Nature, vol. 8(1), pages 1-10, December.
    3. Yangju Lin & Tatiana B. Kouznetsova & Chia-Chih Chang & Stephen L. Craig, 2020. "Enhanced polymer mechanical degradation through mechanochemically unveiled lactonization," Nature Communications, Nature, vol. 11(1), pages 1-9, December.
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