Bioinspired Hydrogen Bonds of Nucleobases Enable Programmable Morphological Transformations of Mixed Nanostructures

Biological systems enable the efficient implementation of various functions by segregating responsive biomacromolecules or assemblies in disparate compartments, which is highly fascinating and desired by materials scientists. However, it is still challenging to elegantly modulate the responsive behaviors of mixed assemblies in synthetic polymeric systems owing to the lack of delicately responsive nanostructures. Herein, bioinspired complementary hydrogen bonding interactions of nucleobases are harnessed to achieve the programmable morphological transformations of mixed nanostructures from cellulose-grafted bottlebrush polymers. Both adenine- and thymine-containing cellulose-grafted-polymers (Cell-g-PAAc and Cell-g-PTAc) were successfully synthesized by using reversible addition-fragmentation chain transfer (RAFT) polymerization. Furthermore, self-assembly of Cell-g-PAAc and Cell-g-PTAc produces well-defined spherical assemblies MA and MT without the discernible particle- partide interaction. In contrast, MA and MT undergo distinct morphological transformations with the introduction of linear diblock copolymers containing complementary nucleobases. By utilizing the novel properties of nanostructures from cellulose-grafted bottlebrush polymers, it is feasible to achieve the selective responsiveness of mixed nanostructures based on complementary hydrogen bonds of nucleobases. This work presents an efficient bioinspired strategy to elegantly modulate the responsive behaviors of mixed nanostructures, providing a cue for fabricating advanced synthetic stimuli-responsive materials.

Automated summary

This study utilizes bioinspired complementary hydrogen bonding interactions to achieve programmable morphological transformations of mixed nanostructures from cellulose-grafted bottlebrush polymers. This work provides an efficient bioinspired strategy to elegantly modulate the responsive behaviors of mixed nanostructures.