Journal
CHEMISTRY-A EUROPEAN JOURNAL
Volume 26, Issue 44, Pages 9982-9990Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/chem.202001505
Keywords
F-19 MRI; amphiphilic copolymer; fluorinated monomers; oxygen sensing; polyacrylates
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Funding
- National Science Foundation [CHE-1847362]
- 3M
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Effective diagnosis of disease and its progression can be aided by(19)F magnetic resonance imaging (MRI) techniques. Specifically, the inherent sensitivity of the spin-lattice relaxation time (T-1) of(19)F nuclei to oxygen partial pressure makes(19)F MRI an attractive non-invasive approach to quantify tissue oxygenation in a spatiotemporal manner. However, there are only few materials with the adequate sensitivity to be used as oxygen-sensitive(19)F MRI agents at clinically relevant field strengths. Motivated by the limitations in current technologies, we report highly fluorinated monomers that provide a platform approach to realize water-soluble, partially fluorinated copolymers as(19)F MRI agents with the required sensitivity to quantify solution oxygenation at clinically relevant magnetic field strengths. The synthesis of a systematic library of partially fluorinated copolymers enabled a comprehensive evaluation of copolymer structure-property relationships relevant to(19)F MRI. The highest-performing material composition demonstrated a signal-to-noise ratio that corresponded to an apparent(19)F density of 220 mm, which surpasses the threshold of 126 mm(19)F required for visualization on a three Tesla clinical MRI. Furthermore, theT(1)of these high performing materials demonstrated a linear relationship with solution oxygenation, with oxygen sensitivity reaching 240x10(-5) mmHg(-1)s(-1). The relationships between material composition and(19)F MRI performance identified herein suggest general structure-property criteria for the further improvement of modular, water-soluble(19)F MRI agents for quantifying oxygenation in environments relevant to medical imaging.
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