Identifying routes for transferring spin polarization from parahydrogen to protic solvents

Repeatable hyperpolarization of high concentrations of mobile protons (>6 M) using parahydrogen in protic methanol/water mixtures is reported here. Different ammonium buffers with increasing mobile proton concentrations were added to an IrCl(COD)(IMes) catalyst in the presence of pyridine. We rea...

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Veröffentlicht in:Chemical communications (Cambridge, England) England), 2024-11, Vol.6 (94), p.13923-13926
Hauptverfasser: Vaneeckhaute, Ewoud, Tyburn, Jean-Max, Kempf, James G, Martens, Johan A, Breynaert, Eric
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Sprache:eng
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Zusammenfassung:Repeatable hyperpolarization of high concentrations of mobile protons (>6 M) using parahydrogen in protic methanol/water mixtures is reported here. Different ammonium buffers with increasing mobile proton concentrations were added to an IrCl(COD)(IMes) catalyst in the presence of pyridine. We reach a maximum molar polarization of 1.79 mM at 6 mT. Field-cycling experiments in an 18.8 T detection field distinguished two solvent polarization transfer pathways: chemical exchange with labile protons from ammonia and cross-relaxation with pyridine aromatic protons. Repeatable hyperpolarization of high proton concentrations (>6 M) is accomplished at low-field by polarization transfer from p-H 2 to hydroxyl protons via chemical exchange or cross-relaxation using hyperpolarized ammonia or pyridine respectively.
ISSN:1359-7345
1364-548X
1364-548X
DOI:10.1039/d4cc03468f