Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 59, Issue 1, Pages 418-423Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201910506
Keywords
acetate; heteronuclei; hyperpolarization; parahydrogen; SABRE-SHEATH
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Funding
- NSF [CHE-1905341, CHE-1904780, CHE-1416432, CHE-1665090, CHE-1836308]
- REU funding from the NSF/DoD ASSURE Program [DMR-1757954]
- SIUC MTC
- OSPA
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Herein, we demonstrate direct C-13 hyperpolarization of C-13-acetate via signal amplification by reversible exchange (SABRE). The standard SABRE homogeneous catalyst [Ir-IMes; [IrCl(COD)(IMes)], (IMes=1,3-bis(2,4,6-trimethylphenyl), imidazole-2-ylidene; COD=cyclooctadiene)] was first activated in the presence of an auxiliary substrate (pyridine) in alcohol. Following addition of sodium 1-C-13-acetate, parahydrogen bubbling within a microtesla magnetic field (i.e. under conditions of SABRE in shield enables alignment transfer to heteronuclei, SABRE-SHEATH) resulted in positive enhancements of up to approximate to 100-fold in the (CNMR)-C-13 signal compared to thermal equilibrium at 9.4T. The present results are consistent with a mechanism of direct transfer of spin order from parahydrogen to C-13 spins of acetate weakly bound to the catalyst, under conditions of fast exchange with respect to the C-13 acetate resonance, but we find that relaxation dynamics at microtesla fields alter the optimal matching from the traditional SABRE-SHEATH picture. Further development of this approach could lead to new ways to rapidly, cheaply, and simply hyperpolarize a broad range of substrates (e.g. metabolites with carboxyl groups) for various applications, including biomedical NMR and MRI of cellular and in vivo metabolism.
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