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Subgroup 1 Multivalent Supramolecular Self-Assembly

2022/1/20 18:19:17

在过去的数十年中,超分子化学经历了迅猛发展。其中,基于配位键优异的方向性和可控性,配位自组装已经成为构筑二维和三维超分子结构的有效手段。迄今为止,此领域涌现出大量的大环和多面体组装体,然后多数结构的复杂度和组装的精准度依然不及生物大分子,由此导致功能的精妙程度也远远低于生物体系。围绕以上挑战,我们团队致力于针对以下三个方面开展了系统研究:

(1)我们发展了基于多臂配体的多重配位自组装策略,实现了二维和三维超分子结构的精准构筑。这些具有精确结构的超分子可以进一步组装成为规则有序的纳米结构,并且具有独特的性质。

(2)复杂超分子组装的不可控性和表征手段的缺乏已严重制约了此领域在功能方向的探索。针对此挑战,我们团队发展了基于多维度质谱和扫描隧道显微镜(STM)的表征技术,突破了具有大分子量和弱相互作用的超分子结构表征瓶颈。同时我们将探索制备级质谱与STM的一体化装置研制,即pMS-STM,此装置可实现大分子结构的原位可视化表征。

(3)基于多重配位自组装和独特的表征手段,我们致力于具有分子层次精准度的新材料开发,探索的范围包括主客体化学、分子识别、反应调控、仿生催化、模板合成以及生物医学。


The past few decades have seen a significant growth in the field of supramolecular chemistry. Due to its highly directional and predictable feature, coordination-driven self-assembly has evolved into a well-established methodology for constructing 2D and 3D supramolecules. Up to date, this field has matured in the context of a large variety of macrocycles and polyhedra, which however, still suffered from a lack of complexity and thus were unable to reach the high level of functionality found in biological systems. With the goal of assembling structures with comparable complexity as biomacromolecules and desired function, we push the limits of coordination-driven self-assembly through the following three aspects.

(1) Design and synthesize multitopic building blocks to construct giant 2D and 3D supramolecular architectures via multivalent coordination-driven self-assembly. Such constructs with precise-controlled shapes and sizes are able to hierarchically assemble into ordered nanostructures with specific properties. During our study of supramolecular chemistry, we believe that an understanding of the genesis, attributes, and principles of mathematic geometry can provide a foundation for comprehending the structure design of supramolecular chemistry as well as the hierarchical self-assembly.

(2) The characterization of metallo-supramolecules is a longstanding challenge on account of their dynamic nature. We developed multidimensional mass spectrometry along with scanning tunneling spectroscopy for full characterization of metallo-supramolecules. Instead of commercial instrument, we are also interested in developing a 2-in-1 instrument, viz. pMS-STM, by bridging preparative mass spectrometer and ultra-high vacuum scanning tunneling spectroscopy together through ions soft-landing for direct visualization of large assemblies.

(3) Beyond self-assembly, we aim to advance the design and development of new synthetic materials with molecular level precision. We are exploring the applications of these assemblies in diverse fields, such as host-guest chemistry, molecular recognition, reactivity modulation, catalysis, template-directed synthesis and biomedicine.

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