Rapid SABRE catalyst scavenging using functionalized silicas
Rapid SABRE catalyst scavenging using functionalized silicas
In recent years the NMR hyperpolarisation method signal amplification by reversible exchange (SABRE) has been applied to multiple substrates of potential interest for in vivo investigation. Unfortunately, SABRE commonly requires an iridium-containing catalyst that is unsuitable for biomedical applications. This report utilizes inductively coupled plasma-optical emission spectroscopy (ICP-OES) to investigate the potential use of metal scavengers to remove the iridium catalytic species from the solution. The most sensitive iridium emission line at 224.268 nm was used in the analysis. We report the effects of varying functionality, chain length, and scavenger support identity on iridium scavenging efficiency. The impact of varying the quantity of scavenger utilized is reported for the three scavengers with the highest iridium removed from initial investigations: 3-aminopropyl (S1), 3-(imidazole-1-yl)propyl (S4), and 2-(2-pyridyl) (S5) functionalized silica gels. Exposure of an activated SABRE sample (1.6 mg mL−1 of iridium catalyst) to 10 mg of the most promising scavenger (S5) resulted in <1 ppm of iridium being detectable by ICP-OES after 2 min of exposure. We propose that combining the approach described herein with other recently reported approaches, such as catalyst separated-SABRE (CASH-SABRE), would enable the rapid preparation of a biocompatible SABRE hyperpolarized bolus.
Catalyst deactivation, Hyperpolarisation, NMR, SABRE, Solid-supported silicas
Robertson, Thomas
957b392c-1212-4721-bd6d-d1e00ed50a09
Clarke, Leon
ba5030e3-8e17-41f0-9bd1-ec4d120fa4e7
Mewis, Ryan
af7b7548-cf0b-48ba-9aa3-83fcb4a430d9
6 January 2022
Robertson, Thomas
957b392c-1212-4721-bd6d-d1e00ed50a09
Clarke, Leon
ba5030e3-8e17-41f0-9bd1-ec4d120fa4e7
Mewis, Ryan
af7b7548-cf0b-48ba-9aa3-83fcb4a430d9
Robertson, Thomas, Clarke, Leon and Mewis, Ryan
(2022)
Rapid SABRE catalyst scavenging using functionalized silicas.
Molecules, 27 (2), [332].
(doi:10.3390/molecules27020332).
Abstract
In recent years the NMR hyperpolarisation method signal amplification by reversible exchange (SABRE) has been applied to multiple substrates of potential interest for in vivo investigation. Unfortunately, SABRE commonly requires an iridium-containing catalyst that is unsuitable for biomedical applications. This report utilizes inductively coupled plasma-optical emission spectroscopy (ICP-OES) to investigate the potential use of metal scavengers to remove the iridium catalytic species from the solution. The most sensitive iridium emission line at 224.268 nm was used in the analysis. We report the effects of varying functionality, chain length, and scavenger support identity on iridium scavenging efficiency. The impact of varying the quantity of scavenger utilized is reported for the three scavengers with the highest iridium removed from initial investigations: 3-aminopropyl (S1), 3-(imidazole-1-yl)propyl (S4), and 2-(2-pyridyl) (S5) functionalized silica gels. Exposure of an activated SABRE sample (1.6 mg mL−1 of iridium catalyst) to 10 mg of the most promising scavenger (S5) resulted in <1 ppm of iridium being detectable by ICP-OES after 2 min of exposure. We propose that combining the approach described herein with other recently reported approaches, such as catalyst separated-SABRE (CASH-SABRE), would enable the rapid preparation of a biocompatible SABRE hyperpolarized bolus.
Text
molecules-27-00332
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More information
Accepted/In Press date: 21 December 2021
e-pub ahead of print date: 6 January 2022
Published date: 6 January 2022
Additional Information:
Funding Information:
Funding: T.B.R.R. and R.E.M. thank Manchester Metropolitan University for a VC scholarship for T.B.R.R.
Publisher Copyright:
© 2022 by the authors. Licensee MDPI, Basel, Switzerland.
Keywords:
Catalyst deactivation, Hyperpolarisation, NMR, SABRE, Solid-supported silicas
Identifiers
Local EPrints ID: 454235
URI: http://eprints.soton.ac.uk/id/eprint/454235
ISSN: 1420-3049
PURE UUID: 1513cb44-8278-4049-a53f-9d5e68de4e02
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Date deposited: 03 Feb 2022 17:45
Last modified: 17 Mar 2024 04:04
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Author:
Leon Clarke
Author:
Ryan Mewis
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