Aqueous, Heterogeneous para-Hydrogen-Induced 15N Polarization

Liana B. Bales; Kirill V. Kovtunov; Danila A. Barskiy; Roman V. Shchepin; Aaron M. Coffey; Larisa M. Kovtunova; Andrey V. Bukhtiyarov; Matthew A. Feldman; Valerii I. Bukhtiyarov; Eduard Y. Chekmenev; Igor V. Koptyug; Boyd M. Goodson

doi:10.1021/acs.jpcc.7b05912

Aqueous, Heterogeneous para-Hydrogen-Induced ¹⁵N Polarization

Liana B. Bales, Kirill V. Kovtunov, Danila A. Barskiy, Roman V. Shchepin, Aaron M. Coffey, Larisa M. Kovtunova, Andrey V. Bukhtiyarov, Matthew A. Feldman, Valerii I. Bukhtiyarov, Eduard Y. Chekmenev, Igor V. Koptyug, Boyd M. Goodson

Research output: Contribution to journal › Article › peer-review

33 Citations (Scopus)

Abstract

The successful transfer of para-hydrogen-induced polarization to ¹⁵N spins using heterogeneous catalysts in aqueous solutions was demonstrated. Hydrogenation of a synthesized unsaturated ¹⁵N-labeled precursor (neurine) with parahydrogen (p-H₂) over Rh/TiO₂ heterogeneous catalysts yielded a hyperpolarized structural analogue of choline. As a result, ¹⁵N polarization enhancements of over 2 orders of magnitude were achieved for the ¹⁵N-labeled ethyltrimethylammonium ion product in deuterated water at elevated temperatures. Enhanced ¹⁵N NMR spectra were successfully acquired at 9.4 and 0.05 T. Importantly, long hyperpolarization lifetimes were observed at 9.4 T, with a ¹⁵N T₁ of ∼6 min for the product molecules, and the T₁ of the deuterated form exceeded 8 min. Taken together, these results show that this approach for generating hyperpolarized species with extended lifetimes in aqueous, biologically compatible solutions is promising for various biomedical applications.

Original language	English
Pages (from-to)	15304-15309
Number of pages	6
Journal	Journal of Physical Chemistry C
Volume	121
Issue number	28
DOIs	https://doi.org/10.1021/acs.jpcc.7b05912
Publication status	Published - 20 Jul 2017

Keywords

DYNAMIC NUCLEAR-POLARIZATION
FIELD
HYPERPOLARIZED MAGNETIC-RESONANCE
IN-VIVO
MRI
NMR
PARAHYDROGEN-INDUCED POLARIZATION
PASADENA HYPERPOLARIZATION
REVERSIBLE EXCHANGE
SPIN ORDER

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Bales, L. B., Kovtunov, K. V., Barskiy, D. A., Shchepin, R. V., Coffey, A. M., Kovtunova, L. M., Bukhtiyarov, A. V., Feldman, M. A., Bukhtiyarov, V. I., Chekmenev, E. Y., Koptyug, I. V., & Goodson, B. M. (2017). Aqueous, Heterogeneous para-Hydrogen-Induced ¹⁵N Polarization. Journal of Physical Chemistry C, 121(28), 15304-15309. https://doi.org/10.1021/acs.jpcc.7b05912

Bales, Liana B. ; Kovtunov, Kirill V. ; Barskiy, Danila A. ; Shchepin, Roman V. ; Coffey, Aaron M. ; Kovtunova, Larisa M. ; Bukhtiyarov, Andrey V. ; Feldman, Matthew A. ; Bukhtiyarov, Valerii I. ; Chekmenev, Eduard Y. ; Koptyug, Igor V. ; Goodson, Boyd M. / Aqueous, Heterogeneous para-Hydrogen-Induced ¹⁵N Polarization. In: Journal of Physical Chemistry C. 2017 ; Vol. 121, No. 28. pp. 15304-15309.

@article{c76b5e4026624b39850c4423ba71cef0,

title = "Aqueous, Heterogeneous para-Hydrogen-Induced 15N Polarization",

abstract = "The successful transfer of para-hydrogen-induced polarization to 15N spins using heterogeneous catalysts in aqueous solutions was demonstrated. Hydrogenation of a synthesized unsaturated 15N-labeled precursor (neurine) with parahydrogen (p-H2) over Rh/TiO2 heterogeneous catalysts yielded a hyperpolarized structural analogue of choline. As a result, 15N polarization enhancements of over 2 orders of magnitude were achieved for the 15N-labeled ethyltrimethylammonium ion product in deuterated water at elevated temperatures. Enhanced 15N NMR spectra were successfully acquired at 9.4 and 0.05 T. Importantly, long hyperpolarization lifetimes were observed at 9.4 T, with a 15N T1 of ∼6 min for the product molecules, and the T1 of the deuterated form exceeded 8 min. Taken together, these results show that this approach for generating hyperpolarized species with extended lifetimes in aqueous, biologically compatible solutions is promising for various biomedical applications.",

keywords = "DYNAMIC NUCLEAR-POLARIZATION, FIELD, HYPERPOLARIZED MAGNETIC-RESONANCE, IN-VIVO, MRI, NMR, PARAHYDROGEN-INDUCED POLARIZATION, PASADENA HYPERPOLARIZATION, REVERSIBLE EXCHANGE, SPIN ORDER",

author = "Bales, {Liana B.} and Kovtunov, {Kirill V.} and Barskiy, {Danila A.} and Shchepin, {Roman V.} and Coffey, {Aaron M.} and Kovtunova, {Larisa M.} and Bukhtiyarov, {Andrey V.} and Feldman, {Matthew A.} and Bukhtiyarov, {Valerii I.} and Chekmenev, {Eduard Y.} and Koptyug, {Igor V.} and Goodson, {Boyd M.}",

note = "Publisher Copyright: {\textcopyright} 2017 American Chemical Society.",

year = "2017",

month = jul,

day = "20",

doi = "10.1021/acs.jpcc.7b05912",

language = "English",

volume = "121",

pages = "15304--15309",

journal = "Journal of Physical Chemistry C",

issn = "1932-7447",

publisher = "American Chemical Society",

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Aqueous, Heterogeneous para-Hydrogen-Induced ¹⁵N Polarization. / Bales, Liana B.; Kovtunov, Kirill V.; Barskiy, Danila A.; Shchepin, Roman V.; Coffey, Aaron M.; Kovtunova, Larisa M.; Bukhtiyarov, Andrey V.; Feldman, Matthew A.; Bukhtiyarov, Valerii I.; Chekmenev, Eduard Y.; Koptyug, Igor V.; Goodson, Boyd M.

In: Journal of Physical Chemistry C, Vol. 121, No. 28, 20.07.2017, p. 15304-15309.

Research output: Contribution to journal › Article › peer-review

TY - JOUR

T1 - Aqueous, Heterogeneous para-Hydrogen-Induced 15N Polarization

AU - Bales, Liana B.

AU - Kovtunov, Kirill V.

AU - Barskiy, Danila A.

AU - Shchepin, Roman V.

AU - Coffey, Aaron M.

AU - Kovtunova, Larisa M.

AU - Bukhtiyarov, Andrey V.

AU - Feldman, Matthew A.

AU - Bukhtiyarov, Valerii I.

AU - Chekmenev, Eduard Y.

AU - Koptyug, Igor V.

AU - Goodson, Boyd M.

PY - 2017/7/20

Y1 - 2017/7/20

N2 - The successful transfer of para-hydrogen-induced polarization to 15N spins using heterogeneous catalysts in aqueous solutions was demonstrated. Hydrogenation of a synthesized unsaturated 15N-labeled precursor (neurine) with parahydrogen (p-H2) over Rh/TiO2 heterogeneous catalysts yielded a hyperpolarized structural analogue of choline. As a result, 15N polarization enhancements of over 2 orders of magnitude were achieved for the 15N-labeled ethyltrimethylammonium ion product in deuterated water at elevated temperatures. Enhanced 15N NMR spectra were successfully acquired at 9.4 and 0.05 T. Importantly, long hyperpolarization lifetimes were observed at 9.4 T, with a 15N T1 of ∼6 min for the product molecules, and the T1 of the deuterated form exceeded 8 min. Taken together, these results show that this approach for generating hyperpolarized species with extended lifetimes in aqueous, biologically compatible solutions is promising for various biomedical applications.

AB - The successful transfer of para-hydrogen-induced polarization to 15N spins using heterogeneous catalysts in aqueous solutions was demonstrated. Hydrogenation of a synthesized unsaturated 15N-labeled precursor (neurine) with parahydrogen (p-H2) over Rh/TiO2 heterogeneous catalysts yielded a hyperpolarized structural analogue of choline. As a result, 15N polarization enhancements of over 2 orders of magnitude were achieved for the 15N-labeled ethyltrimethylammonium ion product in deuterated water at elevated temperatures. Enhanced 15N NMR spectra were successfully acquired at 9.4 and 0.05 T. Importantly, long hyperpolarization lifetimes were observed at 9.4 T, with a 15N T1 of ∼6 min for the product molecules, and the T1 of the deuterated form exceeded 8 min. Taken together, these results show that this approach for generating hyperpolarized species with extended lifetimes in aqueous, biologically compatible solutions is promising for various biomedical applications.

KW - DYNAMIC NUCLEAR-POLARIZATION

KW - FIELD

KW - HYPERPOLARIZED MAGNETIC-RESONANCE

KW - IN-VIVO

KW - MRI

KW - NMR

KW - PARAHYDROGEN-INDUCED POLARIZATION

KW - PASADENA HYPERPOLARIZATION

KW - REVERSIBLE EXCHANGE

KW - SPIN ORDER

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U2 - 10.1021/acs.jpcc.7b05912

DO - 10.1021/acs.jpcc.7b05912

M3 - Article

C2 - 29238438

AN - SCOPUS:85025806660

VL - 121

SP - 15304

EP - 15309

JO - Journal of Physical Chemistry C

JF - Journal of Physical Chemistry C

SN - 1932-7447

IS - 28

ER -

Aqueous, Heterogeneous para-Hydrogen-Induced ¹⁵N Polarization

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