Molecular hydrogen and catalytic combustion in the production of hyperpolarized 83Kr and 129Xe MRI contrast agents

Rogers, Nicola J.; Hill-Casey, Fraser; Stupic, Karl F.; Six, Joseph S.; Lesbats, Cl�mentine; Rigby, Sean P.; Fraissard, Jacques; Pavlovskaya, Galina E.; Meersmann, Thomas

Abstract

Hyperpolarized (hp) 83Kr is a promising MRI contrast agent for the diagnosis of pulmonary diseases affecting the surface of the respiratory zone. However, the distinct physical properties of 83Kr that enable unique MRI contrast also complicate the production of hp 83Kr. This work presents a previously unexplored approach in the generation of hp 83Kr that can likewise be used for the production of hp 129Xe. Molecular nitrogen, typically used as buffer gas in spin-exchange optical pumping (SEOP), was replaced by molecular hydrogen without penalty for the achievable hyperpolarization. In this particular study, the highest obtained nuclear spin polarizations were P = 29% for 83Kr and P = 63% for 129Xe. The results were reproduced over many SEOP cycles despite the laser-induced on-resonance formation of rubidium hydride (RbH). Following SEOP, the H2 was reactively removed via catalytic combustion without measurable losses in hyperpolarized spin state of either 83Kr or 129Xe. Highly spin-polarized 83Kr can now be purified for the first time, to our knowledge, to provide high signal intensity for the advancement of in vivo hp 83Kr MRI. More generally, a chemical reaction appears as a viable alternative to the cryogenic separation process, the primary purification method of hp 129Xe for the past 2 1/2 decades. The inherent simplicity of the combustion process will facilitate hp 129Xe production and should allow for on-demand continuous flow of purified and highly spin-polarized 129Xe.

Citation

Rogers, N. J., Hill-Casey, F., Stupic, K. F., Six, J. S., Lesbats, C., Rigby, S. P., …Meersmann, T. (2016). Molecular hydrogen and catalytic combustion in the production of hyperpolarized 83Kr and 129Xe MRI contrast agents. Proceedings of the National Academy of Sciences, 113(12), 3164-3168. https://doi.org/10.1073/pnas.1600379113

• Journal Article Type: Article
• Acceptance Date: Jan 29, 2016
• Online Publication Date: Mar 9, 2016
• Publication Date: Mar 22, 2016
• Deposit Date: Mar 10, 2016
• Publicly Available Date: Mar 10, 2016
• Journal: Proceedings of the National Academy of Sciences of the United States of America
• Print ISSN: 0027-8424
• Electronic ISSN: 1091-6490
• Publisher: National Academy of Sciences
• Peer Reviewed: Peer Reviewed
• Volume: 113
• Issue: 12
• Pages: 3164-3168
• DOI: https://doi.org/10.1073/pnas.1600379113
• Keywords: spin exchange optical pumping, hyperpolarized noble gas contrast agents, cryogenic separation, chemical looping combustion, catalytic hydrogen oxidation
• Public URL: https://nottingham-repository.worktribe.com/output/780962
• Publisher URL: http://www.pnas.org/content/early/2016/03/08/1600379113
• Related Public URLs: http://www.pnas.org/