(15)N Hyperpolarization of Imidazole-(15)N2 for Magnetic Resonance pH Sensing via SABRE-SHEATH.
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Abstract
(15)N nuclear spins of imidazole-(15)N2 were hyperpolarized using NMR signal amplification by reversible exchange in shield enables alignment transfer to heteronuclei (SABRE-SHEATH). A (15)N NMR signal enhancement of ∼2000-fold at 9.4 T is reported using parahydrogen gas (∼50% para-) and ∼0.1 M imidazole-(15)N2 in methanol:aqueous buffer (∼1:1). Proton binding to a (15)N site of imidazole occurs at physiological pH (pKa ∼ 7.0), and the binding event changes the (15)N isotropic chemical shift by ∼30 ppm. These properties are ideal for in vivo pH sensing. Additionally, imidazoles have low toxicity and are readily incorporated into a wide range of biomolecules. (15)N-Imidazole SABRE-SHEATH hyperpolarization potentially enables pH sensing on scales ranging from peptide and protein molecules to living organisms.
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Shchepin, Roman V, Danila A Barskiy, Aaron M Coffey, Thomas Theis, Fan Shi, Warren S Warren, Boyd M Goodson, Eduard Y Chekmenev, et al. (2016). (15)N Hyperpolarization of Imidazole-(15)N2 for Magnetic Resonance pH Sensing via SABRE-SHEATH. ACS Sens, 1(6). pp. 640–644. 10.1021/acssensors.6b00231 Retrieved from https://hdl.handle.net/10161/15446.
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Warren S. Warren
Our work focuses on the design and application of what might best be called novel pulsed techniques, using controlled radiation fields to alter dynamics. The heart of the work is chemical physics, and most of what we do is ultrafast laser spectroscopy or nuclear magnetic resonance. It generally involves an intimate mixture of theory and experiment: recent publications are roughly an equal mix of pencil- and-paper theory, computer calculations with our workstations, and experiments. Collaborations also play an important role, particularly for medical applications.
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