Thermosetting supramolecular polymerization of compartmentalized DNA fibers with stereo sequence and length control
Thermosetting supramolecular polymerization of compartmentalized DNA fibers with stereo sequence and length control
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DOI：
10.1016/j.chempr.2021.05.022
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发表时间：
2021-06
期刊：
影响因子：
23.5
通讯作者：
Michael D. Dore;Tuan Trinh;Marlo L. Zorman;D. Rochambeau;Casey M. Platnich;Pengfei Xu;Xin Luo;J. Remington;V. Toader;G. Cosa;Jianing Li;H. Sleiman
中科院分区：
文献类型：
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作者：
Michael D. Dore;Tuan Trinh;Marlo L. Zorman;D. Rochambeau;Casey M. Platnich;Pengfei Xu;Xin Luo;J. Remington;V. Toader;G. Cosa;Jianing Li;H. Sleiman
DNA纳米结构是高度可寻址的，与生物系统兼容，但通常需要数百个独特的链进行组装。另一方面，大自然可以通过划分过程来从相同的构建块组装复杂的结构：将分子组装成子组件，并将这些子组件在多个长度尺度上组合在一起。受此过程的启发，我们报告的DNA聚合物共轭物组装通过一个独特的热驱动的分层机制，形成纤维显示块的不同DNA序列沿着其聚合轴。这些一维“热固性”DNA纤维保留了预先组装的片段中编程的区室化。纤维段的长度控制也通过预组装的圆柱形胶束的凝胶纯化来实现。重要的是，我们表明，疏水核心的立体化学序列可以被放大到DNA纤维中的独特的形态特征。分子动力学模拟被用来模拟结构，并阐明立体化学序列如何体现在不同的纤维-纤维相互作用。
DNA nanostructures are highly addressable and compatible with biological systems but often require hundreds of unique strands for their assembly. On the other hand, nature can assemble complex structures from identical building blocks by compartmentalizing the process: assembling molecules into sub-components and bringing these together across multiple length scales. Inspired by this process, we report DNA-polymer conjugates that assemble through a unique heat-driven hierarchical mechanism to form fibers displaying blocks of different DNA sequences along their axis of polymerization. These one-dimensional "thermoset" DNA fibers retain the compartmentalization programmed in the pre-assembled segments. Length control over fiber segments is also achieved through gel purification of pre-assembled cylindrical micelles. Importantly, we show that the stereochemical sequence of the hydrophobic core can be amplified into distinctive morphological traits in the DNA fibers. Molecular dynamics simulations are used to model the structure and elucidate how stereochemical sequence manifests itself in different fiber-fiber interactions.