The solution self-assembly of amphiphilic block copolymers has facilitated the preparation of a wide variety of nano-objects of diverse morphology. Nucleobase-containing block copolymers and their nanostructures have been extensively studied for their ability to mimic DNA and for their specific and complementary hydrogen-bonding interactions. Recently, our group has reported a novel supramolecular self-assembly process for tuneable growth of well-defined anisotropic worm-like micelles from isotropic spherical micelle seeds, based on H-bonding interactions between complementary adenine (A)- and thymine (T)-containing block copolymers. Based on our initial study, the universal character of this hierarchical self-assembly mechanism has been further extended herein toward transforming nucleobase-containing block copolymer vesicles, prepared <i>via </i>aqueous reversible addition-fragmentation chain-transfer (RAFT)-mediated polymerization-induced self-assembly (PISA), as well as core–shell bottlebrush polymers (BBPs) synthesized <i>via </i>a combination of ring-opening metathesis polymerization (ROMP) and RAFT polymerization, following a “grafting-from” approach. In both cases, unique higher-order morphologies could be accessed and their characteristics could be precisely tuned by controlling the degree of polymerization and molar ratio of complementary A- and T-functionalized copolymers. Overall, our work highlights the potential of nucleobase-containing block copolymer nano-objects as platforms for understanding fundamental self-assembly processes and their future application in catalysis, sensing, and nanomedicine.

Controlling the supramolecular self-assembly of nucleobase-containing block copolymer nanostructures

ACS Fall 2021

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