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Macromolecular metamorphosis via stimulus-induced transformations of polymer architecture

Nature Chemistry volume 9, pages 817823 (2017) | Download Citation

Abstract

Macromolecular architecture plays a pivotal role in determining the properties of polymers. When designing polymers for specific applications, it is not only the size of a macromolecule that must be considered, but also its shape. In most cases, the topology of a polymer is a static feature that is inalterable once synthesized. Using reversible-covalent chemistry to prompt the disconnection of chemical bonds and the formation of new linkages in situ, we report polymers that undergo dramatic topological transformations via a process we term macromolecular metamorphosis. Utilizing this technique, a linear amphiphilic block copolymer or hyperbranched polymer undergoes ‘metamorphosis’ into comb, star and hydrophobic block copolymer architectures. This approach was extended to include a macroscopic gel which transitioned from a densely and covalently crosslinked network to one with larger distances between the covalent crosslinks when heated. These architectural transformations present an entirely new approach to ‘smart’ materials.

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Acknowledgements

This material is based on work supported by the National Science Foundation (DMR-1606410).

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Affiliations

  1. George & Josephine Butler Polymer Research Laboratory, Center for Macromolecular Science & Engineering, Department of Chemistry, University of Florida, PO Box 117200, Gainesville, USA

    • Hao Sun
    • , Christopher P. Kabb
    • , Yuqiong Dai
    • , Megan R. Hill
    • , Ion Ghiviriga
    • , Abhijeet P. Bapat
    •  & Brent S. Sumerlin

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Contributions

H.S., A.P.B and B.S.S. conceived and designed the experiments; H.S., C.P.K. and Y.D. performed the experiments; I.G. helped perform and analyse DOSY experiments; H.S., C.P.K. and M.R.H. conducted theoretical calculations; H.S., C.P.K. and M.R.H. analysed and discussed the data; H.S. and C.P.K. prepared all the figures; H.S., B.S.S., C.P.K. and M.R.H. co-wrote the paper.

Competing interests

The authors declare no competing financial interests.

Corresponding author

Correspondence to Brent S. Sumerlin.

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DOI

https://doi.org/10.1038/nchem.2730

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