Disproportionation and self-sorting in molecular encapsulation

Disproportionation and self-sorting in molecular encapsulation
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DOI:
10.1073/pnas.0809903106
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发表时间:
2009-06-30
影响因子:
11.1
通讯作者:
Rebek, Julius, Jr.
Rebek, Julius, Jr.
中科院分区:
综合性期刊1区
文献类型:
--
作者:
Ajami, Dariush;Hou, Jun-Li;Rebek, Julius, Jr.

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自组装胶囊是由多个合成亚基通过弱分子间力结合在一起的纳米级结构。它们充当宿主结构,可以完全包围具有适当大小、形状和化学表面的小分子客人。就像它们的生物对应物,多聚酶和受体一样,胶囊的亚基通常是相同的,并导致高度对称的同质组装。在生物和合成系统中,结构的微小变化都是可以容忍的,并导致具有略微不同识别特性的异质组装。合成胶囊是动态的,寿命从几毫秒到几小时不等,并且可以在环境条件下对溶液中的平衡小分子进行直接光谱观察。我们在这里报道了由两种不同结构组成的杂化胶囊的组装,这两种结构都能够通过氢键形成自己的同质胶囊。这些杂化体表现出与母体胶囊明显不同的宿主特性,这表明其他胶囊可能从看似无关的模块中产生,这些模块具有曲面和丰富的氢键能力。
Self-assembled capsules are nanoscale structures made up of multiple synthetic subunits held together by weak intermolecular forces. They act as host structures that can completely surround small molecule guests of the appropriate size, shape and chemical surface. Like their biological counterparts, multimeric enzymes and receptors, the subunits of the capsules are generally identical, and lead to homomeric assemblies of high symmetry. In both biological and synthetic systems small variations in structures are tolerated and lead to heteromeric assemblies with slightly different recognition properties. The synthetic capsules are dynamic, with lifetimes from milliseconds to hours, and allow the direct spectroscopic observation of smaller molecules inside, under ambient conditions at equilibrium in solution. We report here the assembly of hybrid capsules made up of 2 very different structures, both capable of forming their own homomeric capsules through hydrogen bonding. These hybrids exhibit host properties that differ markedly from the parent capsules, and suggest that other capsules may emerge from seemingly unrelated modules that have curved surfaces and are rich in hydrogen bonding capabilities.