Rayner, Peter John orcid.org/0000-0002-6577-4117, Gillions, Joseph, Hannibal, Valentin et al. (2 more authors) (2021) Hyperpolarisation of weakly binding N-heterocycles using Signal Amplification by Reversible Exchange. Chemical Science. pp. 5910-5917. ISSN 2041-6539
Abstract
Signal Amplification by Reversible Exchange (SABRE) is a catalytic method for improving the detection of molecules by magnetic resonance spectroscopy. It achieves this by simultaneously binding the target substrate (sub) and para-hydrogen to a metal centre. To date, sterically large substrates are relatively inacessable to SABRE due to their weak binding leading to catalyst destabilisation. We overcome this problem here through a simple co-ligand strategy that allows the hyperpolarisation of a range of weakly binding and sterically encumbered N-heterocycles. The resulting 1H NMR signal size is increased by up to 1400 times relative to their more usual Boltzmann controlled levels at 400 MHz. Hence, a significant reduction in scan time is achieved. The SABRE catalyst in these systems takes the form [IrX(H)2(NHC)(sulfoxide)(sub)] where X = Cl, Br or I. These complexes are shown to undergo very rapid ligand exchange and lower temperatures dramatically improves the efficiency of these SABRE catalysts.
Metadata
Item Type: | Article |
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Authors/Creators: |
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Copyright, Publisher and Additional Information: | © 2021 The Author(s). Published by the Royal Society of Chemistry. |
Dates: |
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Institution: | The University of York |
Academic Units: | The University of York > Faculty of Sciences (York) > Chemistry (York) |
Funding Information: | Funder Grant number MEDICAL RESEARCH COUNCIL (MRC) MR/M008991/1 WELLCOME TRUST 098335/Z/12/Z |
Depositing User: | Pure (York) |
Date Deposited: | 30 Mar 2021 10:40 |
Last Modified: | 26 Nov 2024 00:49 |
Published Version: | https://doi.org/10.1039/d0sc06907h |
Status: | Published |
Refereed: | Yes |
Identification Number: | 10.1039/d0sc06907h |
Open Archives Initiative ID (OAI ID): | oai:eprints.whiterose.ac.uk:172703 |