Department of Chemistry and Chemical Biology, Northeastern University, Boston, Massachusetts 02115, United States.
Polymer Program, Institute of Materials Science, University of Connecticut, Storrs, Connecticut 06269, United States.
J Am Chem Soc. 2020 Jun 10;142(23):10297-10301. doi: 10.1021/jacs.0c03806. Epub 2020 Jun 1.
Herein, we report the DNA-mediated self-assembly of bivalent bottlebrush polymers, a process akin to the step-growth polymerization of small molecule monomers. In these "condensation reactions", the polymer serves as a steric guide to limit DNA hybridization in a fixed direction, while the DNA serves as a functional group equivalent, connecting complementary brushes to form well-defined, one-dimensional nanostructures. The polymerization was studied using spectroscopy, microscopy, and scattering techniques and was modeled numerically. The model made predictions of the degree of polymerization and size distribution of the assembled products, and suggested the potential for branching at hybridization junctions, all of which were confirmed experimentally. This study serves as a theoretical basis for the polymer-assembly approach which has the potential to open up new possibilities for suprapolymers with controlled architecture, macromonomer sequence, and end-group functionalities.
在此，我们报告了二价瓶刷聚合物的 DNA 介导自组装，这一过程类似于小分子单体的逐步聚合。在这些“缩合反应”中，聚合物作为空间导向基团限制 DNA 沿固定方向杂交，而 DNA 则作为功能基团等价物，连接互补的刷以形成具有良好定义的一维纳米结构。聚合反应使用光谱学、显微镜和散射技术进行了研究，并进行了数值模拟。该模型对组装产物的聚合度和尺寸分布进行了预测，并提出了在杂交连接处可能发生支化的可能性，所有这些都通过实验得到了证实。这项研究为聚合物组装方法提供了理论基础，该方法有可能为具有可控结构、大分子单体序列和端基功能的超聚合物开辟新的可能性。
