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首页> 外文期刊>Journal of the American Chemical Society >Responsive Supramolecular Polymer Metallogel Constructed by Orthogonal Coordination-Driven Self-Assembly and Host/Guest Interactions
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Responsive Supramolecular Polymer Metallogel Constructed by Orthogonal Coordination-Driven Self-Assembly and Host/Guest Interactions

机译：正交配位驱动的自组装和宿主/客体相互作用构建的响应性超分子聚合物金属

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摘要

An emerging strategy for the fabrication of advanced supramolecular materials is the use of hierarchical self-assembly techniques wherein multiple orthogonal interactions between molecular precursors can produce new species with attractive properties. Herein, we unify the spontaneous formation of metal-ligand bonds with the host/guest chemistry of crown ethers to deliver a 3D supramolecular polymer network (SPN). Specifically, we have prepared a highly directional dipyridyl donor decorated with a benzo-21-crown-7 moiety that undergoes coordination-driven self-assembly with a complementary organoplatinum acceptor to furnish hexagonal metallacycles. These hexagons subsequently polymerize into a supramolecular network upon the addition of a bisammonium salt due to the formation of pseudorotaxane linkages between the crown ether and ammonium moieties. At high concentrations, the resulting 3D SPN becomes a gel comprising many cross-linked metallohexagons. Notably, thermo- and cation-induced gel-sol transitions are found to be completely reversible, reflecting the dynamic and tunable nature of such supramolecular materials. As such, these results demonstrate the structural complexity that can be obtained when carefully controlling multiple interactions in a hierarchical fashion, in this case coordination and host/guest chemistry, and the interesting dynamic properties associated with the materials thus obtained.
机译：制造高级超分子​​材料的一种新兴策略是使用分层自组装技术，其中分子前体之间的多个正交相互作用可以产生具有有吸引力特性的新物种。在本文中，我们将冠状醚的主体/客体化学与金属-配体键的自发形成统一，以提供3D超分子聚合物网络（SPN）。具体来说，我们准备了一个高度定向的二吡啶基供体，装饰有一个苯并21冠7部分，该配体通过与互补有机铂受体的配位驱动自组装来提供六角形金属环。由于在冠醚和铵部分之间形成假轮烷键，因此在添加双铵盐后，这些六边形随后聚合成超分子网络。在高浓度下，所得的3D SPN成为包含许多交联的金属六边形的凝胶。值得注意的是，发现热和阳离子诱导的凝胶-溶胶转变是完全可逆的，反映了这种超分子材料的动态和可调谐性质。这样，这些结果证明了当以分级方式仔细地控制多个相互作用时，在这种情况下的配位和主体/客体化学，以及与由此获得的材料相关的令人感兴趣的动态特性，可以得到结构的复杂性。

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  • 来源
    《Journal of the American Chemical Society》 |2014年第12期|4460-4463|共4页
  • 作者

    Xuzhou Yan; Timothy R. Cook; J. Bryant Pollock; Peifa Wei; Yanyan Zhang; Yihua Yu; Feihe Huang; Peter J. Stang;

  • 作者单位

    State Key Laboratory of Chemical Engineering, Department of Chemistry, Zhejiang University, Hangzhou, Zhejiang 310027, P. R. China;

    Department of Chemistry, University of Utah, 315 South 1400 East, Room 2020, Salt Lake City, Utah 84112, United States;

    Department of Chemistry, University of Utah, 315 South 1400 East, Room 2020, Salt Lake City, Utah 84112, United States;

    State Key Laboratory of Chemical Engineering, Department of Chemistry, Zhejiang University, Hangzhou, Zhejiang 310027, P. R. China;

    Shanghai Key Laboratory of Magnetic Resonance, Department of Physics, East China Normal University, Shanghai 200062, P. R. China;

    Shanghai Key Laboratory of Magnetic Resonance, Department of Physics, East China Normal University, Shanghai 200062, P. R. China;

    State Key Laboratory of Chemical Engineering, Department of Chemistry, Zhejiang University, Hangzhou, Zhejiang 310027, P. R. China;

    Department of Chemistry, University of Utah, 315 South 1400 East, Room 2020, Salt Lake City, Utah 84112, United States;

  • 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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