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Force-induced activation of covalent bonds in mechanoresponsive polymeric materials

机译：力诱导机械响应性聚合物材料中共价键的活化

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摘要

Mechanochemical transduction enables an extraordinary range of physiological processes such as the sense of touch, hearing, balance, muscle contraction, and the growth and remodelling of tissue and bone. Although biology is replete with materials systems that actively and functionally respond to mechanical stimuli, the default mechanochemical reaction of bulk polymers to large external stress is the unselective scission of covalent bonds, resulting in damage or failure. An alternative to this degradation process is the rational molecular design of synthetic materials such that mechanical stress favourably alters material properties. A few mechanosensitive polymers with this property have been developed; but their active response is mediated through non-covalent processes, which may limit the extent to which properties can be modified and the long-term stability in structural materials. Previously, we have shown with dissolved polymer strands incorporating mechanically sensitive chemical groups-so-called mechanophores-that the directional nature of mechanical forces can selectively break and re-form covalent bonds. We now demonstrate that such force-induced covalent-bond activation can also be realized with mechanophore-linked elastomeric and glassy polymers, by using a mechanophore that changes colour as it undergoes a reversible electrocyclic ring-opening reaction under tensile stress and thus allows us to directly and locally visualize the mechanochemical reaction. We find that pronounced changes in colour and fluorescence emerge with the accumulation of plastic deformation, indicating that in these polymeric materials the transduction of mechanical force into the ring-opening reaction is an activated process. We anticipate that force activation of covalent bonds can serve as a general strategy for the development of new mechanophore building blocks that impart polymeric materials with desirable functionalities ranging from damage sensing to fully regenerative self-healing.
机译：机械化学转导可实现各种生理过程，例如触觉，听觉，平衡，肌肉收缩以及组织和骨骼的生长和重塑。尽管生物学中充满了对机械刺激进行主动和功能响应的材料系统，但本体聚合物对大外部应力的默认机械化学反应是共价键的非选择性断裂，从而导致破坏或破坏。降解过程的替代方法是合理设计合成材料的分子，以使机械应力有利地改变材料性能。已经开发出一些具有这种性能的机械敏感性聚合物。但它们的主动反应是通过非共价过程介导的，这可能会限制可改性特性的程度以及结构材料的长期稳定性。以前，我们已经证明，结合了机械敏感的化学基团的溶解的聚合物链（所谓的力学基团），机械力的方向性可以选择性地破坏并重新形成共价键。现在，我们证明，通过使用在张力下经历可逆的电环开环反应时颜色会改变的机制，也可以通过与机制结合的弹性体和玻璃状聚合物实现这种力诱导的共价键活化。直接和局部可视化机械化学反应。我们发现随着塑性变形的积累，颜色和荧光发生了明显变化，这表明在这些聚合物材料中，机械力向开环反应的传递是一个激活的过程。我们预计，共价键的力激活可以作为开发新的机制载体的一般策略，这些机制赋予聚合物材料所需的功能，从损伤检测到完全再生的自我修复。

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  • 来源
    《Nature》 |2009年第7243期|68-72|共5页
  • 作者

    Douglas A. Davis; Andrew Hamilton; Jinglei Yang; Lee D. Cremar; Dara Van Gough; Stephanie L. Potisek; Mitchell T. Ong; Paul V. Braun; Todd J. Martinez; Scott R. White; Jeffrey S. Moore; Nancy R. Sottos;

  • 作者单位

    Department of Chemistry, University of Illinois at Urbana-Champaign, Illinois 61801, USA;

    Department of Mechanical Science and Engineering, University of Illinois at Urbana-Champaign, Illinois 61801, USA;

    The Beckman Institute, University of Illinois at Urbana-Champaign, Illinois 61801, USA School of Mechanical and Aerospace Engineering, Nanyang Technological University, Singapore (J.Y.) Department of Chemistry, Stanford University, Stanford, California, USA (T.J.M.);

    Department of Chemistry, University of Illinois at Urbana-Champaign, Illinois 61801, USA;

    Department of Materials Science and Engineering, University of Illinois at Urbana-Champaign, Illinois 61801, USA;

    Department of Chemistry, University of Illinois at Urbana-Champaign, Illinois 61801, USA;

    Department of Chemistry, University of Illinois at Urbana-Champaign, Illinois 61801, USA;

    Department of Chemistry, University of Illinois at Urbana-Champaign, Illinois 61801, USA The Beckman Institute, University of Illinois at Urbana-Champaign, Illinois 61801, USA Department of Materials Science and Engineering, University of Illinois at Urbana-Champaign, Illinois 61801, USA;

    Department of Chemistry, University of Illinois at Urbana-Champaign, Illinois 61801, USA The Beckman Institute, University of Illinois at Urbana-Champaign, Illinois 61801, USA School of Mechanical and Aerospace Engineering, Nanyang Technological University, Singapore (J.Y.) Department of Chemistry, Stanford University, Stanford, California, USA (T.J.M.);

    The Beckman Institute, University of Illinois at Urbana-Champaign, Illinois 61801, USA Department of Aerospace Engineering, University of Illinois at Urbana-Champaign, Illinois 61801, USA;

    Department of Chemistry, University of Illinois at Urbana-Champaign, Illinois 61801, USA The Beckman Institute, University of Illinois at Urbana-Champaign, Illinois 61801, USA Department of Materials Science and Engineering, University of Illinois at Urbana-Champaign, Illinois 61801, USA;

    The Beckman Institute, University of Illinois at Urbana-Champaign, Illinois 61801, USA Department of Materials Science and Engineering, University of Illinois at Urbana-Champaign, Illinois 61801, USA;

  • 收录信息 美国《科学引文索引》(SCI);美国《工程索引》(EI);美国《生物学医学文摘》(MEDLINE);美国《化学文摘》(CA);
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