Brush-First and ROMP-Out with Functional (Macro)monomers: Method Development, Structural Investigations, and Applications of an Expanded Brush-Arm Star Polymer Platform
Name
nihms-1037657.pdf
Description
Accepted version
Size
1.32 MB
Format
Adobe PDF
Checksum (MD5)
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Author(s)
Golder, Matthew R
Nguyen, Hung VanThanh.
Oldenhuis, Nathan
Grundler, Julian
Park, Ellane J.
Johnson, Jeremiah A.
Date Issued
December 2018
Journal
Macromolecules
Publisher
American Chemical Society (ACS)
Citation
Golder, Matthew R. et al. “Brush-First and ROMP-Out with Functional (Macro)monomers: Method Development, Structural Investigations, and Applications of an Expanded Brush-Arm Star Polymer Platform.” Macromolecules 51 (2018): 9861-9870 © 2018 The Author(s)
Version
Author's final manuscript
Abstract
The efficient synthesis of complex functional polymeric nanomaterials is often challenging. Ru-initiated ring-opening metathesis polymerization (ROMP) of multivalent macromonomers followed by cross-linking to form brush-arm star (BASP) polymers enables access to well-defined nanostructures with diverse functionality. This "brush-first" method leaves active Ru in the BASP microgel core, which could potentially be used in a subsequent "ROMP-out" (RO) step to introduce further modifications to the BASP structure via the addition of (macro)monomers. Here, we study this RO approach in depth. The efficiency of RO is assessed for a variety of BASP compositions using a combination of inductively coupled plasma mass spectrometry and gel permeation chromatography. To demonstrate the modularity of the RO process, arylboronic acid-functionalized BASPs were prepared; uptake of these RO-BASPs into hypersialylated cancer cells was enhanced relative to non-functionalized BASPs as determined by flow cytometry and fluorescence microscopy. In addition, the self-assembly of miktoarm BASPs prepared via brush-first and RO with different macromonomers is demonstrated. The combination of brush-first ROMP with RO provides a simple, modular strategy for access to a wide array of functional nanomaterials.
MIT Department
Massachusetts Institute of Technology. Department of Chemistry
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DOI of Published Version
https://doi.org/10.1021/ACS.MACROMOL.8B01966
