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Tunable, biodegradable grafting-from glycopolypeptide bottlebrush polymers

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Listed:
  • Zachary S. Clauss

    (University of Utah)

  • Casia L. Wardzala

    (University of Utah)

  • Austin E. Schlirf

    (University of Utah)

  • Nathaniel S. Wright

    (University of Utah)

  • Simranpreet S. Saini

    (University of Utah)

  • Bibiana Onoa

    (Howard Hughes Medical Institute University of California Berkeley)

  • Carlos Bustamante

    (Howard Hughes Medical Institute University of California Berkeley
    University of California Berkeley
    University of California
    Lawrence Berkeley National Laboratory)

  • Jessica R. Kramer

    (University of Utah
    University of Utah)

Abstract

The cellular glycocalyx and extracellular matrix are rich in glycoproteins and proteoglycans that play essential physical and biochemical roles in all life. Synthetic mimics of these natural bottlebrush polymers have wide applications in biomedicine, yet preparation has been challenged by their high grafting and glycosylation densities. Using one-pot dual-catalysis polymerization of glycan-bearing α-amino acid N-carboxyanhydrides, we report grafting-from glycopolypeptide brushes. The materials are chemically and conformationally tunable where backbone and sidechain lengths were precisely altered, grafting density modulated up to 100%, and glycan density and identity tuned by monomer feed ratios. The glycobrushes are composed entirely of sugars and amino acids, are non-toxic to cells, and are degradable by natural proteases. Inspired by native lipid-anchored proteoglycans, cholesterol-modified glycobrushes were displayed on the surface of live human cells. Our materials overcome long-standing challenges in glycobrush polymer synthesis and offer new opportunities to examine glycan presentation and multivalency from chemically defined scaffolds.

Suggested Citation

  • Zachary S. Clauss & Casia L. Wardzala & Austin E. Schlirf & Nathaniel S. Wright & Simranpreet S. Saini & Bibiana Onoa & Carlos Bustamante & Jessica R. Kramer, 2021. "Tunable, biodegradable grafting-from glycopolypeptide bottlebrush polymers," Nature Communications, Nature, vol. 12(1), pages 1-11, December.
    • Handle: RePEc:nat:natcom:v:12:y:2021:i:1:d:10.1038_s41467-021-26808-5
    DOI: 10.1038/s41467-021-26808-5
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    References listed on IDEAS

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    1. Timothy J. Deming, 1997. "Facile synthesis of block copolypeptides of defined architecture," Nature, Nature, vol. 390(6658), pages 386-389, November.
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