Amphiphilic-DNA Platform for the Design of Crystalline Frameworks with Programmable Structure and Functionality
Amphiphilic-DNA Platform for the Design of Crystalline Frameworks with Programmable Structure and Functionality
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DOI：
10.1021/jacs.8b09143
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发表时间：
2018-11-14
影响因子：
15
通讯作者：
Di Michele, Lorenzo
中科院分区：
文献类型：
--
作者：
Brady, Ryan A.;Brooks, Nicholas J.;Di Michele, Lorenzo
功能性、有序的纳米结构框架的可靠制备将改变许多新兴技术的游戏规则，从能量存储到纳米医学。DNA纳米技术以核酸优异的分子识别能力为基础，沿着其易于合成和广泛的可用功能化，被广泛认为是合理设计纳米结构材料的主要途径。然而，制备具有可编程结构和功能的结晶DNA框架仍然是一个挑战。在这里，我们展示了简单的两亲性DNA基序的潜力，被称为“C-stars”，作为一个通用的平台，用于设计可编程的DNA晶体。与全DNA材料不同，其结构取决于单个构建块的精确分子细节，C星的自组装是由其拓扑结构和对称性唯一控制的。利用这种强大的自组装原理，我们设计了一系列拓扑结构相同，但结构和化学上不同的C-星，遵循一锅反应自组装成高度多孔，功能，结晶框架。简单的设计变化使我们能够微调晶格参数，从而控制大分子在框架内的分配，嵌入可以诱导等温分解的响应基序，并包括化学部分以特异性和可逆地捕获靶蛋白。
The reliable preparation of functional, ordered, nano-structured frameworks would be a game changer for many emerging technologies, from energy storage to nanomedicine. Underpinned by the excellent molecular recognition of nucleic acids, along with their facile synthesis and breadth of available functionalizations, DNA nanotechnology is widely acknowledged as a prime route for the rational design of nanostructured materials. Yet, the preparation of crystalline DNA frameworks with programmable structure and functionality remains a challenge. Here we demonstrate the potential of simple amphiphilic DNA motifs, dubbed "C-stars", as a versatile platform for the design of programmable DNA crystals. In contrast to all-DNA materials, in which structure depends on the precise molecular details of individual building blocks, the self-assembly of C-stars is controlled uniquely by their topology and symmetry. Exploiting this robust self assembly principle, we design a range of topologically identical, but structurally and chemically distinct C-stars that following a one-pot reaction self-assemble into highly porous, functional, crystalline frameworks. Simple design variations allow us to finetune the lattice parameter and thus control the partitioning of macromolecules within the frameworks, embed responsive motifs that can induce isothermal disassembly, and include chemical moieties to capture target proteins specifically and reversibly.