"Giant surfactants" created by the fast and efficient functionalization of a DNA tetrahedron with a temperature-responsive polymer.
"Giant surfactants" created by the fast and efficient functionalization of a DNA tetrahedron with a temperature-responsive polymer.
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DOI：
10.1021/nn402642a
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发表时间：
2013-10
期刊：
影响因子：
17.1
通讯作者：
Thomas R. Wilks;J. Bath;J. W. de Vries;Jeffery E. Raymond;A. Herrmann;A. Turberfield;R. O’Reilly
中科院分区：
文献类型：
--
作者：
Thomas R. Wilks;J. Bath;J. W. de Vries;Jeffery E. Raymond;A. Herrmann;A. Turberfield;R. O’Reilly
采用铜催化叠氮-炔环加成反应（CuAAC）合成了具有温度响应性的聚（N-异丙基丙烯酰胺）（聚（NIPAM））和高疏水性聚（苯乙烯）等聚合物嵌段的DNA嵌段共聚物（DBC）。在低DNA浓度下，在有机溶剂中，并且在没有任何固体支持物的情况下，实现了异常高的产率。DBC的DNA片段仍然能够进行序列特异性杂交：它被用来组装一个精确定义的纳米结构，一个DNA四面体，具有悬垂的聚（NIPAM）片段。在过量的聚（NIPAM）均聚物的存在下，四面体-聚（NIPAM）缀合物在40 °C（均聚物从溶液中沉淀的温度）下成核形成大的、明确限定的纳米颗粒。通过动态光散射和cryoTEM观察这些复合纳米颗粒，并通过AFM成像证实了它们的混合性质。由于四面体的大有效表面积，仅需要非常低浓度的缀合物就可以观察到这种表面活性剂样行为。
Copper catalyzed azide-alkyne cycloaddition (CuAAC) was employed to synthesize DNA block copolymers (DBCs) with a range of polymer blocks including temperature-responsive poly(N-isoproylacrylamide) (poly(NIPAM)) and highly hydrophobic poly(styrene). Exceptionally high yields were achieved at low DNA concentrations, in organic solvents, and in the absence of any solid support. The DNA segment of the DBC remained capable of sequence-specific hybridization: it was used to assemble a precisely defined nanostructure, a DNA tetrahedron, with pendant poly(NIPAM) segments. In the presence of an excess of poly(NIPAM) homopolymer, the tetrahedron-poly(NIPAM) conjugate nucleated the formation of large, well-defined nanoparticles at 40 °C, a temperature at which the homopolymer precipitated from solution. These composite nanoparticles were observed by dynamic light scattering and cryoTEM, and their hybrid nature was confirmed by AFM imaging. As a result of the large effective surface area of the tetrahedron, only very low concentrations of the conjugate were required in order for this surfactant-like behavior to be observed.