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Cationic, Anionic, and Amphoteric Dual pH/Temperature-Responsive Degradable Microgels via Self-Assembly of Functionalized Oligomeric Precursor Polymers

  • Eva Mueller
    Eva Mueller
    Department of Chemical Engineering, McMaster University, 1280 Main St. W, Hamilton, Ontario, Canada L8S 4L7
    More by Eva Mueller
  • Sebastian Himbert
    Sebastian Himbert
    Department of Physics and Astronomy, McMaster University, 1280 Main St. W, Hamilton, Ontario, Canada L8S 4M1
  • Madeline J. Simpson
    Madeline J. Simpson
    Department of Chemical Engineering, McMaster University, 1280 Main St. W, Hamilton, Ontario, Canada L8S 4L7
  • Markus Bleuel
    Markus Bleuel
    NIST Center for Neutron Research, National Institute of Standards and Technology, Gaithersburg, Maryland 20899-3460, United States
    Department of Materials Science and Engineering, University of Maryland, College Park, Maryland 20742-2115, United States
  • Maikel C. Rheinstadter
    Maikel C. Rheinstadter
    Department of Physics and Astronomy, McMaster University, 1280 Main St. W, Hamilton, Ontario, Canada L8S 4M1
  • , and 
  • Todd Hoare*
    Todd Hoare
    Department of Chemical Engineering, McMaster University, 1280 Main St. W, Hamilton, Ontario, Canada L8S 4L7
    *Email: [email protected]
    More by Todd Hoare
Cite this: Macromolecules 2021, 54, 1, 351–363
Publication Date (Web):December 29, 2020
https://doi.org/10.1021/acs.macromol.0c02304
Copyright © 2020 American Chemical Society

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    Abstract

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    Multiresponsive smart materials with the capacity to reversibly change properties (i.e., size, charge) upon the application of more than one stimulus (i.e., temperature, pH) offer potential in numerous biotechnology and biomedical applications. However, their typical lack of degradability limits their potential in vivo use. Herein, we demonstrate the use of an aqueous thermally driven self-assembly approach based on hydrazide- and aldehyde-functionalized poly(N-isopropylacrylamide) (PNIPAM) oligomers functionalized with pH-ionizable cationic or anionic comonomers for fabricating degradable temperature/pH dual-responsive microgels. The self-assembled microgels show properties analogous to conventional cationic or anionic PNIPAM microgels, retaining their thermal responsiveness while exhibiting pH-driven swelling upon functional comonomer ionization. Amphoteric microgels can also be produced by mixing cationic- and anionic-functionalized precursor polymers during the self-assembly process that reproduce the high-pH/low-pH parabolic swelling response observed in conventional amphoteric microgels. Coupling the precise dual-responsive swelling responses achievable with the degradability of the hydrazone cross-links, self-assembled charged PNIPAM microgels offer potential for improved performance in drug delivery applications requiring dual pH/temperature-specific delivery (e.g. infection sites or cancer).

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.macromol.0c02304.

    • 1H NMR spectra of the acrylate hydrazide monomer and the four charged hydrazide or aldehyde-functionalized precursor polymers, cloud point curves over the full scanned temperature range using UV–vis spectrophotometry, and SANS/USANS data for same charge cross-linker/seed polymer and opposite charge cross-linker/seed polymer microgel assemblies are provided (PDF)

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