The self-organization of pre-assembled aggregates is an efficient stepwise strategy for fabricating nanostructures with a second level of hierarchy. Herein, we report that anisotropic spindle-like micelles, self-assembled from polypeptide graft copolymers with rigid backbones, can serve as ideal pre-assembled subunits for constructing one-dimensional materials with hierarchical structures. By adding organic solvents and dialyzing against water, reactive points can be generated at the ends of the spindle-like micelles, which subsequently drive the anisotropic micelles to grow as rods in a chain and eventually self-assemble into hierarchical nanowires in a stepwise manner. The second self-assembly step is a hierarchical process that resembles step polymerization. Hierarchical structures can be precisely synthesized by this new type of polymerization. These nanostructures can be tailored by the activity of the reactive points, which depends on the nature of the solvent and the molecular architecture.
Self-assembly behavior of mixture systems containing poly(γ-benzyl-L-glutamate)-poly(ethylene glycol) graft (PBLG-g-PEG) and block (PBLG-b-PEG) copolymers in aqueous solution was investigated by both experiments and computer simulations. Pure graft copolymers self-assembled into vesicles, and pure block copolymers aggregated into spherical micelles or vesicles, while, for the mixture systems, hybrid cylindrical micelles were observed. In addition to the experimental observations, self-consistent field theory (SCFT) simulations were performed on the self-assembly behavior of graft/block copolymer mixtures. Simulation results reproduced the morphological transitions observed in the experiments. Moreover, from the SCFT simulations, the chain distributions of copolymers in the aggregates were obtained. For the hybrid cylindrical micelles, block copolymers were found to mainly locate at the ends of aggregates, which prevents the fusion of cylinders to vesicles. By combining experimental findings with simulation results, the mechanism regarding the morphological transition of the aggregates formed by graft/block copolymer mixtures is proposed.
We discovered that micelles of a thermo-responsive polypeptide-based copolymer are able to direct growth of barium carbonate (BaCO(3)) in the form of nanobelts. The BaCO(3) nanobelts tend to grow around a formed crystal, and curl into a spiral superstructure.
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