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Thermoresponsive Triblock Copolymers as Widely Applicable 19F Magnetic Resonance Imaging Tracers

  • Kristyna Kolouchova*
    Kristyna Kolouchova
    Polymer Chemistry and Biomaterials Group, Centre of Macromolecular Chemistry, Department of Organic and Macromolecular Chemistry, Ghent University, Krijgslaan 281, S4-Bis, 9000Ghent, Belgium
    *Email: [email protected]
  • Ondrej Groborz
    Ondrej Groborz
    Institute of Macromolecular Chemistry, Czech Academy of Sciences, Heyrovského sq. 2, 162 06Prague 6, Czech Republic
    Institute of Biophysics and Informatics, Charles University, First Faculty of Medicine, Salmovská 1, 120 00Prague 2, Czech Republic
    Institute of Organic Chemistry and Biochemistry, Czech Academy of Sciences, Flemingovo sq. 2, 160 00Prague 6, Czech Republic
  • Miroslav Slouf
    Miroslav Slouf
    Institute of Macromolecular Chemistry, Czech Academy of Sciences, Heyrovského sq. 2, 162 06Prague 6, Czech Republic
  • Vit Herynek
    Vit Herynek
    Center for Advanced Preclinical Imaging (CAPI), First Faculty of Medicine, Charles University, Salmovská 3, 120 00Prague 2, Czech Republic
    More by Vit Herynek
  • Laurens Parmentier
    Laurens Parmentier
    Polymer Chemistry and Biomaterials Group, Centre of Macromolecular Chemistry, Department of Organic and Macromolecular Chemistry, Ghent University, Krijgslaan 281, S4-Bis, 9000Ghent, Belgium
  • David Babuka
    David Babuka
    Institute of Macromolecular Chemistry, Czech Academy of Sciences, Heyrovského sq. 2, 162 06Prague 6, Czech Republic
    More by David Babuka
  • Zulfiya Cernochova
    Zulfiya Cernochova
    Institute of Macromolecular Chemistry, Czech Academy of Sciences, Heyrovského sq. 2, 162 06Prague 6, Czech Republic
  • Filip Koucky
    Filip Koucky
    Department of Inorganic Chemistry, Faculty of Science, Charles University, Hlavova 8, 128 43Praha 2, Czech Republic
    More by Filip Koucky
  • Ondrej Sedlacek
    Ondrej Sedlacek
    Department of Physical and Macromolecular Chemistry, Faculty of Science, Charles University, 128 40Prague 2, Czech Republic
  • Martin Hruby
    Martin Hruby
    Institute of Macromolecular Chemistry, Czech Academy of Sciences, Heyrovského sq. 2, 162 06Prague 6, Czech Republic
    More by Martin Hruby
  • Richard Hoogenboom
    Richard Hoogenboom
    Supramolecular Chemistry Group, Department of Organic and Macromolecular Chemistry, Centre of Macromolecular Chemistry, Ghent University, Krijgslaan 281-S4, 9000Ghent, Belgium
  • , and 
  • Sandra Van Vlierberghe*
    Sandra Van Vlierberghe
    Polymer Chemistry and Biomaterials Group, Centre of Macromolecular Chemistry, Department of Organic and Macromolecular Chemistry, Ghent University, Krijgslaan 281, S4-Bis, 9000Ghent, Belgium
    *Email: [email protected]
Cite this: Chem. Mater. 2022, 34, 24, 10902–10916
Publication Date (Web):December 12, 2022
https://doi.org/10.1021/acs.chemmater.2c02589
Copyright © 2022 American Chemical Society

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    Abstract

    Abstract Image

    Fluorine-19 magnetic resonance imaging (19F MRI) has emerged as a promising noninvasive diagnostic tool, broadening the diagnostic possibilities of commonly used proton MRI. Despite the potential of 19F MRI, an ideal tracer paving the way toward the entry of this method into common medical practice is yet to be developed. In this study, we report on a series of polymeric systems based on thermoresponsive poly[N-(2,2-difluoroethyl)acrylamide] (PDFEA), a polymer considered to be an ideal tracer for 19F MRI. The described systems are designed as BAB triblock copolymers, where B corresponds to thermoresponsive PDFEA blocks and A is a hydrophilic poly(ethylene glycol) block. These BAB triblock copolymers are able to form nanoparticles in dilute aqueous solutions, which undergo a transition into physically cross-linked hydrogels upon increasing the polymer concentration. Since thermoresponsive particle- and hydrogel-based systems are applicable in a wide range of biomedical applications, we created a diagnostic system with potential therapeutic properties (theranostic) as a widely tunable platform through straightforward synthesis while serving a multitude of applications. We analyzed the effect of the BAB block ratio on the self-assembly, thermoresponsiveness, and mechanical properties of the studied hydrogels, together with their suitability for 19F MRI. Finally, their biocompatibility was assessed on a relevant cell line.

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    Supporting Information

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.chemmater.2c02589.

    • SEC figures; NMR spectra; CTA content in prepared polymers; DLS, rheology; and turbidimetry figures; TEM and SEM micrographs; 19F relaxations (T1 and T2); MRS and MRI data; and cytotoxicity assay (PDF)

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    Most electronic Supporting Information files are available without a subscription to ACS Web Editions. Such files may be downloaded by article for research use (if there is a public use license linked to the relevant article, that license may permit other uses). Permission may be obtained from ACS for other uses through requests via the RightsLink permission system: http://pubs.acs.org/page/copyright/permissions.html.

    Cited By

    This article is cited by 1 publications.

    1. Kristyna Kolouchova, Ondrej Groborz, Vit Herynek, Oleg V. Petrov, Jan Lang, David Dunlop, Laurens Parmentier, Anna Szabó, David Schaubroeck, Peter Adriaensens, Sandra Van Vlierberghe. Cell-Interactive Gelatin-Based 19F MRI Tracers: An In Vitro Proof-of-Concept Study. Chemistry of Materials 2024, 36 (1) , 183-196. https://doi.org/10.1021/acs.chemmater.3c01574

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