Low-Cost High-Pressure Clinical-Scale 50% Parahydrogen Generator Using Liquid Nitrogen at 77 K | Sciact - CRIS-system of Boreskov Institute of Catalysis

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

Journal

Analytical Chemistry
ISSN: 0003-2700 , E-ISSN: 1520-6882

Output data

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

Tags

Liquids, Copper, Catalysts, Nuclear magnetic resonance spectroscopy, Polarization

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. ^7,8,9 , 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, Rapid City, South Dakota 57701, United States
2	Department of Chemistry, Integrative Biosciences (Ibio), Wayne State University, Karmanos Cancer Institute (KCI), Detroit, Michigan 48202, United States
3	Department of Chemistry, Biology, and Health Sciences, South Dakota School of Mines and Technology, Rapid City, South Dakota 57701, United States
4	Chemistry and Synthesis Center, National Heart, Lung, and Blood Institute, Bethesda, Maryland 20850, United States
5	Center for Cancer Research, National Cancer Institute, National Institutes of Health, Bethesda, Maryland 20814, United States
6	XeUS Technologies Limited, Lakatamia 2312, Nicosia, Cyprus
7	International Tomography Center, SB RAS, Novosibirsk 630090, Russia
8	Novosibirsk State University, Novosibirsk 630090, Russia
9	Boreskov Institute of Catalysis SB RAS, Novosibirsk 630090, Russia
10	Department of Chemistry and Biochemistry, Southern Illinois University, Carbondale, Illinois 62901, United States
11	Department of Chemistry and Biochemistry and Materials Technology Center, Southern Illinois University, Carbondale, Illinois 62901, United States
12	Russian Academy of Sciences, Moscow 119991, Russia

Funding (13)

1	National Science Foundation	CHE-1416268
2	National Science Foundation	CHE-1416432
3	National Science Foundation	CHE-1905341
4	National Science Foundation	CHE-1904780
5	United States Department of Defense	W81XWH-15-1-0271
6	United States Department of Defense	W81XWH-15-1-0272
7	National Institutes of Health	1R21CA220137
8	National Institute of Biomedical Imaging and Bioengineering	1R01EB029829
9	National Institutes of Health	1R21HL154032-01
10	Ministry of Science and Higher Education of the Russian Federation	075-15-2020-779
11	United States Department of Defense	W81XWH-20-10576
12	United States Department of Defense	W81XWH-20-10578
13	National Institutes of Health	HHSN261200800001E

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 РИНЦ AN PMID OpenAlex

Submitted:	Feb 16, 2021
Accepted:	May 27, 2021
Published online:	Jun 8, 2021
Published print:	Jun 22, 2021

Web of science:	WOS:000665642500014
Scopus:	2-s2.0-85108716669
Elibrary:	46844491
Chemical Abstracts:	2021:1249827
PMID:	34102835
OpenAlex:	W3172259887

DB	Citing
Scopus	29
Web of science	26
Elibrary	21
OpenAlex	31