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(15)N Hyperpolarization of Imidazole-(15)N2 for Magnetic Resonance pH Sensing via SABRE-SHEATH.

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Date
2016-06-24
Authors
Shchepin, Roman V
Barskiy, Danila A
Coffey, Aaron M
Theis, Thomas
Shi, Fan
Warren, Warren S
Goodson, Boyd M
Chekmenev, Eduard Y
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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.
Type
Journal article
Subject
15N
NMR
chemical shift
hyperpolarization
imidazole
pH sensing
parahydrogen
Permalink
https://hdl.handle.net/10161/15446
Published Version (Please cite this version)
10.1021/acssensors.6b00231
Publication Info
Shchepin, Roman V; Barskiy, Danila A; Coffey, Aaron M; Theis, Thomas; Shi, Fan; Warren, Warren S; ... Chekmenev, Eduard Y (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.
This is constructed from limited available data and may be imprecise. To cite this article, please review & use the official citation provided by the journal.
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Scholars@Duke

Theis

Thomas Theis

Assistant Research Professor of Chemistry
Theis' research is at the intersection of Spin Physics and Hyperpolarization Chemistry. It has applications in the study of biochemical dynamics and molecular imaging. The Theis lab drives innovation of magnetic resonance tools and techniques to break the sensitivity limits of NMR  and MRI. The innovations enable i) biochemical structure elucidation with unprecedented limits of detection, and ii) molecular imaging to spy on mole
Warren

Warren S. Warren

James B. Duke Distinguished Professor of Chemistry
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. Collabo
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