Polyoxazoline-Based Bottlebrush and Brush-Arm Star Polymers via ROMP: Syntheses and Applications as Organic Radical Contrast Agents
Name
nihms-1036389.pdf
Description
Accepted version
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920.55 KB
Format
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Author(s)
Alvaradejo, Gabriela Gil
Nguyen, Hung VanThanh
Harvey, Peter
Gallagher, Nolan
Le, Dao
Ottaviani, M. Francesca
Jasanoff, Alan Pradip
Delaittre, Guillaume
Johnson, Jeremiah A.
Date Issued
April 2019
Journal
ACS Macro Letters
Publisher
American Chemical Society (ACS)
Citation
Alvaradejo, Gabriela Gil et al. "Polyoxazoline-Based Bottlebrush and Brush-Arm Star Polymers via ROMP: Syntheses and Applications as Organic Radical Contrast Agents." ACS Macro Letters 8, 4 (April 2019): 473–478 © 2019 American Chemical Society
Version
Author's final manuscript
Abstract
The synthesis of functional poly(2-alkyl-2-oxazoline) (PAOx) copolymers with complex nanoarchitectures using a graft-through ring-opening metathesis polymerization (ROMP) approach is described. First, well-defined norbornene-terminated poly(2-ethyl-2-oxazoline) (PEtOx) macromonomers (MM) were prepared by cationic ring-opening polymerization. ROMP of these MMs produced bottlebrush copolymers with PEtOx side chains. In addition, PEtOx-based branched MMs bearing a terminal alkyne group were prepared and conjugated to an azide-containing bis-spirocyclohexyl nitroxide via Cu-catalyzed azide-alkyne cycloaddition (CuAAC). ROMP of this branched MM, followed by in situ cross-linking, provided PEtOx-based brush-arm star polymers (BASPs) with nitroxide radicals localized at the core-shell interface. These PEtOx-based nitroxide-containing BASPs displayed relaxivity values on par with state-of-the-art polyethylene glycol (PEG)-based nitroxide materials, making them promising as organic radical contrast agents for metal-free magnetic resonance imaging (MRI).
MIT Department
Massachusetts Institute of Technology. Department of Chemistry
Massachusetts Institute of Technology. Department of Biological Engineering
Massachusetts Institute of Technology. Department of Brain and Cognitive Sciences
Massachusetts Institute of Technology. Department of Nuclear Science and Engineering
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DOI of Published Version
https://doi.org/10.1021/acsmacrolett.9b00016
