Department of Chemistry and Center for Self-Assembled Chemical Structures, McGill University, 801 Sherbrooke Street West, Montreal, Quebec H3A 0B8, Canada.
Department of Chemistry, The University of Vermont, Burlington, VT 05405, USA.
Nat Chem. 2018 Feb;10(2):184-192. doi: 10.1038/nchem.2893. Epub 2017 Dec 4.
As colloidal self-assembly increasingly approaches the complexity of natural systems, an ongoing challenge is to generate non-centrosymmetric structures. For example, patchy, Janus or living crystallization particles have significantly advanced the area of polymer assembly. It has remained difficult, however, to devise polymer particles that associate in a directional manner, with controlled valency and recognition motifs. Here, we present a method to transfer DNA patterns from a DNA cage to a polymeric nanoparticle encapsulated inside the cage in three dimensions. The resulting DNA-imprinted particles (DIPs), which are 'moulded' on the inside of the DNA cage, consist of a monodisperse crosslinked polymer core with a predetermined pattern of different DNA strands covalently 'printed' on their exterior, and further assemble with programmability and directionality. The number, orientation and sequence of DNA strands grafted onto the polymeric core can be controlled during the process, and the strands are addressable independently of each other.
随着胶体自组装越来越接近自然系统的复杂性，一个持续的挑战是生成非中心对称结构。例如，有斑点的、两面的或活的结晶粒子极大地推动了聚合物组装领域的发展。然而，设计以可控的价数和识别基序定向结合的聚合物粒子仍然很困难。在这里，我们提出了一种方法，将 DNA 图案从 DNA 笼转移到笼内封装的聚合物纳米粒子中。所得的 DNA 印迹颗粒（DIP）在 DNA 笼内“成型”，由单分散交联聚合物核组成，其外表面有预定图案的不同 DNA 链共价“打印”，并且进一步具有可编程性和方向性组装。在这个过程中可以控制接枝到聚合物核上的 DNA 链的数量、方向和序列，并且可以独立寻址这些链。
