Low-Cost High-Pressure Clinical-Scale 50% Parahydrogen Generator Using Liquid Nitrogen at 77 K

Low-Cost High-Pressure Clinical-Scale 50% Parahydrogen Generator Using Liquid Nitrogen at 77 K Full article

Journal

Analytical Chemistry
ISSN: 0003-2700

Output data

Year: 2021, Volume: 93, Number: 24, Pages: 8476-8483 Pages count : 8 DOI: 10.1021/acs.analchem.1c00716

Authors

Chapman Benjamin ¹ , Joalland Baptiste ² , Meersman Collier ³ , Ettedgui Jessica ⁴ , Swenson Rolf E. ⁴ , Krishna Murali C. ⁵ , Nikolaou Panayiotis ⁶ , Kovtunov Kirill V. ^7,8 , Salnikov Oleg G. ^9,7,8 , Koptyug Igor V. ⁷ , Gemeinhardt Max E. ¹⁰ , Goodson Boyd M. ^10,11 , Shchepin Roman V. ³ , Chekmenev Eduard Y. ^2,12

Affiliations

1	Department of Materials and Metallurgical Engineering, South Dakota School of Mines and Technology, 501 E Street Joseph Street, Rapid City, South Dakota 57701, United States
2	Department of Chemistry, Integrative Biosciences (Ibio), Wayne State University, Karmanos Cancer Institute (KCI), 5101 Cass Avenue, Detroit, Michigan 48202, United States
3	Department of Chemistry, Biology, and Health Sciences, South Dakota School of Mines and Technology, 501 E Street Joseph Street, Rapid City, South Dakota 57701, United States
4	Chemistry and Synthesis Center, National Heart, Lung, and Blood Institute, 9800 Medical Center Drive, Building B, Room #2034, Bethesda, Maryland 20850, United States
5	Center for Cancer Research, National Cancer Institute, National Institutes of Health, 31 Center Drive, Bethesda, Maryland 20814, United States
6	XeUS Technologies Limited, Georgiou Karaiskaki 2A, Lakatamia 2312 Nicosia, Cyprus
7	International Tomography Center, SB RAS, 3A Institutskaya Street, Novosibirsk 630090, Russia
8	Novosibirsk State University, 2 Pirogova Street, Novosibirsk 630090, Russia
9	Boreskov Institute of Catalysis SB RAS, 5 Acad. Lavrentiev Pr., Novosibirsk 630090, Russia
10	Department of Chemistry and Biochemistry, Southern Illinois University, 1245 Lincoln Drive, Carbondale, Illinois 62901, United States
11	Materials Technology Center, Southern Illinois University, 1245 Lincoln Drive, Carbondale, Illinois 62901, United States
12	Russian Academy of Sciences, Leninskiy Prospekt 14, Moscow 119991, Russia

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%.

Chapman B. , Joalland B. , Meersman C. , Ettedgui J. , Swenson R.E. , Krishna M.C. , Nikolaou P. , Kovtunov K.V. , Salnikov O.G. , Koptyug I.V. , Gemeinhardt M.E. , Goodson B.M. , Shchepin R.V. , Chekmenev E.Y.
Low-Cost High-Pressure Clinical-Scale 50% Parahydrogen Generator Using Liquid Nitrogen at 77 K
Analytical Chemistry. 2021. V.93. N24. P.8476-8483. DOI: 10.1021/acs.analchem.1c00716 WOS Scopus OpenAlex

Submitted:	Feb 16, 2021
Accepted:	May 27, 2021
Published print:	Jun 9, 2021

≡ Web of science:	WOS:000665642500014
≡ Scopus:	2-s2.0-85108716669
≡ OpenAlex:	W3172259887