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Mechanical gating of a mechanochemical reaction cascade

Author

Listed:
  • Junpeng Wang

    (Duke University)

  • Tatiana B. Kouznetsova

    (Duke University)

  • Roman Boulatov

    (University of Liverpool)

  • Stephen L. Craig

    (Duke University)

Abstract

Covalent polymer mechanochemistry offers promising opportunities for the control and engineering of reactivity. To date, covalent mechanochemistry has largely been limited to individual reactions, but it also presents potential for intricate reaction systems and feedback loops. Here we report a molecular architecture, in which a cyclobutane mechanophore functions as a gate to regulate the activation of a second mechanophore, dichlorocyclopropane, resulting in a mechanochemical cascade reaction. Single-molecule force spectroscopy, pulsed ultrasonication experiments and DFT-level calculations support gating and indicate that extra force of >0.5 nN needs to be applied to a polymer of gated gDCC than of free gDCC for the mechanochemical isomerization gDCC to proceed at equal rate. The gating concept provides a mechanism by which to regulate stress-responsive behaviours, such as load-strengthening and mechanochromism, in future materials designs.

Suggested Citation

  • 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.
    • Handle: RePEc:nat:natcom:v:7:y:2016:i:1:d:10.1038_ncomms13433
    DOI: 10.1038/ncomms13433
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    Cited by:

    1. Mengqi Du & Hannes A. Houck & Qiang Yin & Yewei Xu & Ying Huang & Yang Lan & Li Yang & Filip E. Du Prez & Guanjun Chang, 2022. "Force–reversible chemical reaction at ambient temperature for designing toughened dynamic covalent polymer networks," Nature Communications, Nature, vol. 13(1), pages 1-9, December.
    2. 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.

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