Research output: Contribution to journal › Article › peer-review
Low-Cost High-Pressure Clinical-Scale 50% Parahydrogen Generator Using Liquid Nitrogen at 77 K. / Chapman, Benjamin; Joalland, Baptiste; Meersman, Collier et al.
In: Analytical Chemistry, Vol. 93, No. 24, 22.06.2021, p. 8476–8483.Research output: Contribution to journal › Article › peer-review
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TY - JOUR
T1 - Low-Cost High-Pressure Clinical-Scale 50% Parahydrogen Generator Using Liquid Nitrogen at 77 K
AU - Chapman, Benjamin
AU - Joalland, Baptiste
AU - Meersman, Collier
AU - Ettedgui, Jessica
AU - Swenson, Rolf E.
AU - Krishna, Murali C.
AU - Nikolaou, Panayiotis
AU - Kovtunov, Kirill V.
AU - Salnikov, Oleg G.
AU - Koptyug, Igor V.
AU - Gemeinhardt, Max E.
AU - Goodson, Boyd M.
AU - Shchepin, Roman V.
AU - Chekmenev, Eduard Y.
N1 - Publisher Copyright: © 2021 American Chemical Society Copyright: Copyright 2021 Elsevier B.V., All rights reserved.
PY - 2021/6/22
Y1 - 2021/6/22
N2 - We report on a robust and low-cost parahydrogen generator design employing liquid nitrogen as a coolant. The core of the generator consists of catalyst-filled spiral copper tubing, which can be pressurized to 35 atm. Parahydrogen fraction >48% was obtained at 77 K with three nearly identical generators using paramagnetic hydrated iron oxide catalysts. Parahydrogen quantification was performed on the fly via benchtop NMR spectroscopy to monitor the signal from residual orthohydrogen-parahydrogen is NMR silent. This real-time quantification approach was also used to evaluate catalyst activation at up to 1.0 standard liter per minute flow rate. The reported inexpensive device can be employed for a wide range of studies employing parahydrogen as a source of nuclear spin hyperpolarization. To this end, we demonstrate the utility of this parahydrogen generator for hyperpolarization of concentrated sodium [1-13C]pyruvate, a metabolic contrast agent under investigation in numerous clinical trials. The reported pilot optimization of SABRE-SHEATH (signal amplification by reversible exchange-shield enables alignment transfer to heteronuclei) hyperpolarization yielded 13C signal enhancement of over 14,000-fold at a clinically relevant magnetic field of 1 T corresponding to approximately 1.2% 13C polarization - if near 100% parahydrogen would have been employed, the reported value would be tripled to 13C polarization of 3.5%.
AB - We report on a robust and low-cost parahydrogen generator design employing liquid nitrogen as a coolant. The core of the generator consists of catalyst-filled spiral copper tubing, which can be pressurized to 35 atm. Parahydrogen fraction >48% was obtained at 77 K with three nearly identical generators using paramagnetic hydrated iron oxide catalysts. Parahydrogen quantification was performed on the fly via benchtop NMR spectroscopy to monitor the signal from residual orthohydrogen-parahydrogen is NMR silent. This real-time quantification approach was also used to evaluate catalyst activation at up to 1.0 standard liter per minute flow rate. The reported inexpensive device can be employed for a wide range of studies employing parahydrogen as a source of nuclear spin hyperpolarization. To this end, we demonstrate the utility of this parahydrogen generator for hyperpolarization of concentrated sodium [1-13C]pyruvate, a metabolic contrast agent under investigation in numerous clinical trials. The reported pilot optimization of SABRE-SHEATH (signal amplification by reversible exchange-shield enables alignment transfer to heteronuclei) hyperpolarization yielded 13C signal enhancement of over 14,000-fold at a clinically relevant magnetic field of 1 T corresponding to approximately 1.2% 13C polarization - if near 100% parahydrogen would have been employed, the reported value would be tripled to 13C polarization of 3.5%.
UR - http://www.scopus.com/inward/record.url?scp=85108716669&partnerID=8YFLogxK
U2 - 10.1021/acs.analchem.1c00716
DO - 10.1021/acs.analchem.1c00716
M3 - Article
C2 - 34102835
AN - SCOPUS:85108716669
VL - 93
SP - 8476
EP - 8483
JO - Analytical Chemistry
JF - Analytical Chemistry
SN - 0003-2700
IS - 24
ER -
ID: 28873897