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„Direct“ 13C Hyperpolarization of 13C-Acetate by MicroTesla NMR Signal Amplification by Reversible Exchange (SABRE)

Publication ,  Journal Article
Gemeinhardt, ME; Limbach, MN; Gebhardt, TR; Eriksson, CW; Eriksson, SL; Lindale, JR; Goodson, EA; Warren, WS; Chekmenev, EY; Goodson, BM
Published in: Advanced Materials
January 1, 2020

Herein, we demonstrate „direct“ 13C hyperpolarization of 13C-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 1-13C-acetate, parahydrogen bubbling within a microtesla magnetic field (i.e. under conditions of SABRE in shield enables alignment transfer to heteronuclei, SABRESHEATH) resulted in positive enhancements of up to ≈ 100- fold in the 13C NMR signal compared to thermal equilibrium at 9.4 T. The present results are consistent with a mechanism of „direct“ transfer of spin order from parahydrogen to 13C spins of acetate weakly bound to the catalyst, under conditions of fast exchange with respect to the 13C 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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Published In

Advanced Materials

DOI

EISSN

1521-4095

ISSN

0935-9648

Publication Date

January 1, 2020

Volume

59

Issue

1

Start / End Page

426 / 431

Related Subject Headings

  • Nanoscience & Nanotechnology
  • 09 Engineering
  • 03 Chemical Sciences
  • 02 Physical Sciences
 

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Gemeinhardt, M. E., Limbach, M. N., Gebhardt, T. R., Eriksson, C. W., Eriksson, S. L., Lindale, J. R., … Goodson, B. M. (2020). „Direct“ 13C Hyperpolarization of 13C-Acetate by MicroTesla NMR Signal Amplification by Reversible Exchange (SABRE). Advanced Materials, 59(1), 426–431. https://doi.org/10.1002/ANGE.201910506
Gemeinhardt, M. E., M. N. Limbach, T. R. Gebhardt, C. W. Eriksson, S. L. Eriksson, J. R. Lindale, E. A. Goodson, W. S. Warren, E. Y. Chekmenev, and B. M. Goodson. “„Direct“ 13C Hyperpolarization of 13C-Acetate by MicroTesla NMR Signal Amplification by Reversible Exchange (SABRE).” Advanced Materials 59, no. 1 (January 1, 2020): 426–31. https://doi.org/10.1002/ANGE.201910506.
Gemeinhardt ME, Limbach MN, Gebhardt TR, Eriksson CW, Eriksson SL, Lindale JR, et al. „Direct“ 13C Hyperpolarization of 13C-Acetate by MicroTesla NMR Signal Amplification by Reversible Exchange (SABRE). Advanced Materials. 2020 Jan 1;59(1):426–31.
Gemeinhardt, M. E., et al. “„Direct“ 13C Hyperpolarization of 13C-Acetate by MicroTesla NMR Signal Amplification by Reversible Exchange (SABRE).” Advanced Materials, vol. 59, no. 1, Jan. 2020, pp. 426–31. Scopus, doi:10.1002/ANGE.201910506.
Gemeinhardt ME, Limbach MN, Gebhardt TR, Eriksson CW, Eriksson SL, Lindale JR, Goodson EA, Warren WS, Chekmenev EY, Goodson BM. „Direct“ 13C Hyperpolarization of 13C-Acetate by MicroTesla NMR Signal Amplification by Reversible Exchange (SABRE). Advanced Materials. 2020 Jan 1;59(1):426–431.
Journal cover image

Published In

Advanced Materials

DOI

EISSN

1521-4095

ISSN

0935-9648

Publication Date

January 1, 2020

Volume

59

Issue

1

Start / End Page

426 / 431

Related Subject Headings

  • Nanoscience & Nanotechnology
  • 09 Engineering
  • 03 Chemical Sciences
  • 02 Physical Sciences