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Edited by David A. Weitz, Harvard University, Cambridge, MA, and approved December 17, 2018 (received for review October 15, 2018)
Significance
Tuning shape, size, and chemical composition elicits a way to mediate function. In soft materials, the establishment of these structure–function relationships has been hampered by the inability to independently control the shape, size, and composition of macromolecules. Here, we establish a synthetic methodology combining a computer-controlled process and two controlled polymerizations to yield macromolecules with any monotonic axisymmetric shape up to 300 nm in size. The methodology has a simple and scalable setup to yield gram quantities of macromolecules from commercially available materials. This approach provides a unique material platform to study the impact of shape, size, and composition of macromolecules.
Abstract
Shape, size, and composition are the 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 that combines reactor engineering principles and controlled polymerizations. Specifically, bottlebrush polymers with conical, ellipsoidal, and concave architectures are synthesized using two orthogonal polymerizations. The chemical versatility is highlighted by the synthesis of a compositional asymmetric cone. The strong agreement between predictions and experiments validates the precision that this methodology offers.
Footnotes
- ↵1To whom correspondence should be addressed. Email: guironne{at}illinois.edu.
Author contributions: D.J.W. and D.G. designed research; D.J.W. performed research; D.J.W. and D.G. analyzed data; and D.J.W. and D.G. wrote the paper.
Conflict of interest statement: An invention disclosure related to this work has been filed: D.G. and D.J.W. filed a US Patent Application, January 2018.
This article is a PNAS Direct Submission.
This article contains supporting information online at www.pnas.org/lookup/suppl/doi:10.1073/pnas.1817745116/-/DCSupplemental.
Published under the PNAS license.
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Macromolecules with programmable shape, size, and chemistry
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