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

使用 77 K 液氮的低成本高压临床级 50% 仲氢发生器

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作者:Benjamin Chapman, Baptiste Joalland, Collier Meersman, Jessica Ettedgui, Rolf E Swenson, Murali C Krishna, Panayiotis Nikolaou, Kirill V Kovtunov, Oleg G Salnikov, Igor V Koptyug, Max E Gemeinhardt, Boyd M Goodson, Roman V Shchepin, Eduard Y Chekmenev

Abstract

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%.

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