Rapid and simple 13C-hyperpolarization by 1H dissolution dynamic nuclear polarization followed by an inline magnetic field inversion
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Accepted version
Author(s)
Type
Journal Article
Abstract
Dissolution dynamic nuclear polarization (dDNP) is a method of choice for preparing hyperpolarized 13C metabolites such as 1-13C-pyruvate used for in vivo applications, including the real-time monitoring of cancer cell metabolism in human patients. The approach consists of transferring the high polarization of electron spins to nuclear spins via microwave irradiation at low temperatures (1.0-1.5 K) and moderate magnetic fields (3.3-7 T). The solid sample is then dissolved and transferred to an NMR spectrometer or MRI scanner for detection in the liquid state. Common dDNP protocols use direct hyperpolarization of 13C spins reaching polarizations of >50% in ∼1-2 h. Alternatively, 1H spins are polarized before transferring their polarization to 13C spins using cross-polarization, reaching polarization levels similar to those of direct DNP in only ∼20 min. However, it relies on more complex instrumentation, requiring highly skilled personnel. Here, we explore an alternative route using 1H dDNP followed by inline adiabatic magnetic field inversion in the liquid state during the transfer. 1H polarizations of >70% in the solid state are obtained in ∼5-10 min. As the hyperpolarized sample travels from the dDNP polarizer to the NMR spectrometer, it goes through a field inversion chamber, which causes the 1H → 13C polarization transfer. This transfer is made possible by the J-coupling between the heteronuclei, which mixes the Zeeman states at zero-field and causes an antilevel crossing. We report liquid-state 13C polarization up to ∼17% for 3-13C-pyruvate and 13C-formate. The instrumentation needed to perform this experiment in addition to a conventional dDNP polarizer is simple and readily assembled.
Date Issued
2023-12-20
Date Acceptance
2023-11-15
Citation
Journal of the American Chemical Society, 2023, 145 (50), pp.27576-27586
ISSN
0002-7863
Publisher
American Chemical Society
Start Page
27576
End Page
27586
Journal / Book Title
Journal of the American Chemical Society
Volume
145
Issue
50
Copyright Statement
Copyright © 2023 American Chemical Society. This document is the Accepted Manuscript version of a Published Work that appeared in final form in
Journal of the American Chemical Society, after peer review and technical editing by the publisher. To access the final edited and published work see 10.1021/jacs.3c09209
Journal of the American Chemical Society, after peer review and technical editing by the publisher. To access the final edited and published work see 10.1021/jacs.3c09209
Identifier
https://www.ncbi.nlm.nih.gov/pubmed/38054954
Publication Status
Published
Coverage Spatial
United States
Date Publish Online
2023-12-06