Shape, size and composition are nature’s most fundamental design features, enabling highly complex functionalities. Despite recent advances, the independent control of shape, size and chemistry of macromolecules remains a synthetic challenge. We report a scalable methodology to produce large well-defined macromolecules with programmable shape, size and chemistry. Specifically, bottlebrush polymers (branched polymers with high branch density all originating from a linear backbone) are synthesized with variable brush length along the backbone. This enables the construction of any axisymmetric shape including: cone, sphere, hourglass, football, and bowtie shapes.<br/>The synthesis is enabled by the combination of reactor engineering principles and controlled polymerizations. One controlled polymerization synthesizes the arms of the bottlebrush (ring opening polymerization or anionic polymerization) and the other polymerizes the backbone of the bottlebrush (ring opening metathesis polymerization). Theoretical derivations, in conjunction with a numerical model, are used to aid in the design and characterization of the shaped macromolecules. We have further characterized the materials through atomic force microscopy (AFM) as well as rheology. Rheological data is further correlated back to Brownian dynamics simulations. This methodology provides a unique opportunity to study the impact of macromolecules shapes.

Flow-enabled control over macromolecule architecture

2019 Spring National Meeting

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