“Direct” <sup>13</sup>C Hyperpolarization of <sup>13</sup>C‐Acetate by MicroTesla NMR Signal Amplification by Reversible Exchange (SABRE)
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- Max E. Gemeinhardt
- Department of Chemistry and Biochemistry Southern Illinois University Carbondale IL 62901 USA
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- Miranda N. Limbach
- Department of Chemistry and Biochemistry Southern Illinois University Carbondale IL 62901 USA
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- Thomas R. Gebhardt
- Department of Chemistry and Biochemistry Southern Illinois University Carbondale IL 62901 USA
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- Clark W. Eriksson
- Department of Biomedical Engineering University of Virginia Charlottesville VA USA
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- Shannon L. Eriksson
- Department of Chemistry Duke University Durham NC USA
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- Jacob R. Lindale
- Department of Chemistry Duke University Durham NC USA
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- Elysia A. Goodson
- Carbondale Community High School Carbondale IL 62901 USA
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- Warren S. Warren
- Department of Chemistry Duke University Durham NC USA
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- Eduard Y. Chekmenev
- Department of Chemistry Karmanos Cancer Institute (KCI) Integrative Biosciences (Ibio) Wayne State University Detroit MI 48202 USA
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- Boyd M. Goodson
- Department of Chemistry and Biochemistry Southern Illinois University Carbondale IL 62901 USA
抄録
<jats:title>Abstract</jats:title><jats:p>Herein, we demonstrate “direct” <jats:sup>13</jats:sup>C hyperpolarization of <jats:sup>13</jats:sup>C‐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‐<jats:sup>13</jats:sup>C‐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 ≈100‐fold in the <jats:sup>13</jats:sup>C 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 <jats:sup>13</jats:sup>C spins of acetate weakly bound to the catalyst, under conditions of fast exchange with respect to the <jats:sup>13</jats:sup>C 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.</jats:p>
収録刊行物
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- Angewandte Chemie International Edition
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Angewandte Chemie International Edition 59 (1), 418-423, 2019-11-14
Wiley
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キーワード
詳細情報 詳細情報について
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- CRID
- 1361981470230920448
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- ISSN
- 15213773
- 14337851
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- データソース種別
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- Crossref