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Hyperpolarized Magnetic Resonance of Exchangeable Protons Using Parahydrogen and Aminosilane

Authors :
Jean-Max Tyburn
Eric Breynaert
Johan A. Martens
Ewoud Vaneeckhaute
David Kilgour
James G. Kempf
Francis Taulelle
Source :
The Journal of Physical Chemistry C. 124:14541-14549
Publication Year :
2020
Publisher :
American Chemical Society (ACS), 2020.

Abstract

Efficient, room temperature hyperpolarisation of exchangeable solvent protons combining parahydrogen (p-H2), ami-nopropyldiethoxymethylsilane (APDMS) and IrCl(COD)(IMES) to generate an active aminosilane-iridium complex, broadens the capabilities of SABRE-type hyperpolarisation of protons. A primary pool of hyperpolarised exchangeable protons transfers its hyperpolarisation to co-solutes with labile protons, partly overcoming the catalytic specificity of SABRE-type spin-transfer catalysis. The silane functionality of APDMS appears to be crucial to the improvement. Their role is unprecedented in p-H2-based hyperpolarisation of nuclear spins and promises to broaden applicability of ultra-sensitive solution-state NMR spectroscopy for the detection and elucidation of molecular behaviors otherwise unde-tectable at conventional sensitivity levels. doi: 10.1021/acs.jpcc.0c01149 Efficient, room temperature hyperpolarisation of exchangeable solvent protons combining parahydrogen (p-H2), ami-nopropyldiethoxymethylsilane (APDMS) and IrCl(COD)(IMES) to generate an active aminosilane-iridium complex, broadens the capabilities of SABRE-type hyperpolarisation of protons. A primary pool of hyperpolarised exchangeable protons transfers its hyperpolarisation to co-solutes with labile protons, partly overcoming the catalytic specificity of SABRE-type spin-transfer catalysis. The silane functionality of APDMS appears to be crucial to the improvement. Their role is unprecedented in p-H2-based hyperpolarisation of nuclear spins and promises to broaden applicability of ultra-sensitive solution-state NMR spectroscopy for the detection and elucidation of molecular behaviors otherwise unde-tectable at conventional sensitivity levels. ispartof: The Journal of Physical Chemistry C: Energy Conversion and Storage, Optical and Electronic Devices, Interfaces, Nanomaterials, and Hard Matter vol:124 issue:27 pages:14541-14549 status: published

Details

ISSN :
19327455 and 19327447
Volume :
124
Database :
OpenAIRE
Journal :
The Journal of Physical Chemistry C
Accession number :
edsair.doi.dedup.....23dfbcb6527bfceb60f72c4e3949de81
Full Text :
https://doi.org/10.1021/acs.jpcc.0c01149