Nitroxyl Modified Tobacco Mosaic Virus as a Metal-Free High-Relaxivity MRI and EPR Active Superoxide Sensor

Molecular Pharmaceutics
Madushani DharmarwardanaJeremiah J Gassensmith

Abstract

Superoxide overproduction is known to occur in multiple disease states requiring critical care; yet, noninvasive detection of superoxide in deep tissue remains a challenge. Herein, we report a metal-free magnetic resonance imaging (MRI) and electron paramagnetic resonance (EPR) active contrast agent prepared by "click conjugating" paramagnetic organic radical contrast agents (ORCAs) to the surface of tobacco mosaic virus (TMV). While ORCAs are known to be reduced in vivo to an MRI/EPR silent state, their oxidation is facilitated specifically by reactive oxygen species-in particular, superoxide-and are largely unaffected by peroxides and molecular oxygen. Unfortunately, single molecule ORCAs typically offer weak MRI contrast. In contrast, our data confirm that the macromolecular ORCA-TMV conjugates show marked enhancement for T1 contrast at low field (<3.0 T) and T2 contrast at high field (9.4 T). Additionally, we demonstrated that the unique topology of TMV allows for a "quenchless fluorescent" bimodal probe for concurrent fluorescence and MRI/EPR imaging, which was made possible by exploiting the unique inner and outer surface of the TMV nanoparticle. Finally, we show TMV-ORCAs do not respond to normal cellular respiration, mi...Continue Reading

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Citations

Apr 16, 2020·Nanoscale·Candace E BenjaminJeremiah J Gassensmith
Apr 7, 2020·Wiley Interdisciplinary Reviews. Nanomedicine and Nanobiotechnology·Mehdi ShahgolzariSteven Fiering
Sep 30, 2020·Annual Review of Virology·Sourabh ShuklaNicole F Steinmetz
Apr 12, 2020·Molecules : a Journal of Synthetic Chemistry and Natural Product Chemistry·Sergey DobryninAlexey Chubarov
Jul 1, 2020·Advanced Drug Delivery Reviews·Young Hun ChungNicole F Steinmetz
Apr 4, 2021·Molecules : a Journal of Synthetic Chemistry and Natural Product Chemistry·Ken-Ichiro MatsumotoMurali C Krishna
May 28, 2021·NPJ Systems Biology and Applications·Yi LiLeonidas Bleris
May 11, 2019·ACS Applied Materials & Interfaces·He HuNicole F Steinmetz
Feb 20, 2019·ACS Applied Materials & Interfaces·Michael A LuzuriagaJeremiah J Gassensmith
Aug 29, 2018·Bioconjugate Chemistry·Raymond P WelchJeremiah J Gassensmith
Sep 23, 2021·Journal of the American Chemical Society·Arezoo ShahrivarkevishahiJeremiah J Gassensmith

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