Towards large-scale steady-state enhanced nuclear magnetization with in situ detection

Publikationstyp:
Zeitschriftenaufsatz
Metadaten:
Autoren
  • John W Blanchard
  • Barbara Ripka
  • Benjamin A Suslick
  • Dario Gelevski
  • Teng Wu
  • Kerstin Muennemann
  • Danila A Barskiy
  • Dmitry Budker
Autoren-URL
https://www.webofscience.com/api/gateway?GWVersion=2&SrcApp=fis-test-1&SrcAuth=WosAPI&KeyUT=WOS:000646697000001&DestLinkType=FullRecord&DestApp=WOS_CPL
DOI
10.1002/mrc.5161
eISSN
1097-458X
Externe Identifier
  • Clarivate Analytics Document Solution ID: WW8YN
  • PubMed Identifier: 33826170
ISSN
0749-1581
Ausgabe der Veröffentlichung
12
Zeitschrift
MAGNETIC RESONANCE IN CHEMISTRY
Schlüsselwörter
  • hyperpolarization
  • in situ detection
  • parahydrogen
  • PHIP
  • SABRE
Paginierung
1208 - 1215
Datum der Veröffentlichung
2021
Status
Published
Titel
Towards large-scale steady-state enhanced nuclear magnetization with in situ detection
Sub types
  • Article
Ausgabe der Zeitschrift
59

Datenquelle: Web of Science (Lite)

Andere Metadatenquellen:
Abstract
<jats:title>Abstract</jats:title><jats:p>Signal amplification by reversible exchange (SABRE) boosts NMR signals of various nuclei enabling new applications spanning from magnetic resonance imaging to analytical chemistry and fundamental physics. SABRE is especially well positioned for continuous generation of enhanced magnetization on a large scale; however, several challenges need to be addressed for accomplishing this goal. Specifically, SABRE requires (i) a specialized catalyst capable of reversible H<jats:sub>2</jats:sub> activation and (ii) physical transfer of the sample from the point of magnetization generation to the point of detection (e.g., a high‐field or a benchtop nuclear magnetic resonance [NMR] spectrometer). Moreover, (iii) continuous parahydrogen bubbling accelerates solvent (e.g., methanol) evaporation, thereby limiting the experimental window to tens of minutes per sample. In this work, we demonstrate a strategy to rapidly generate the best‐to‐date precatalyst (a compound that is chemically modified in the course of the reaction to yield the catalyst) for SABRE, [Ir(IMes)(COD)Cl] (IMes = 1,3‐bis‐[2,4,6‐trimethylphenyl]‐imidazol‐2‐ylidene; COD = cyclooctadiene) via a highly accessible synthesis. Second, we measure hyperpolarized samples using a home‐built zero‐field NMR spectrometer and study the field dependence of hyperpolarization directly in the detection apparatus, eliminating the need to physically move the sample during the experiment. Finally, we prolong the measurement time and reduce evaporation by presaturating parahydrogen with the solvent vapor before bubbling into the sample. These advancements extend opportunities for exploring SABRE hyperpolarization by researchers from various fields and pave the way to producing large quantities of hyperpolarized material for long‐lasting detection of SABRE‐derived nuclear magnetization.</jats:p>
Autoren
  • John W Blanchard
  • Barbara Ripka
  • Benjamin A Suslick
  • Dario Gelevski
  • Teng Wu
  • Kerstin Münnemann
  • Danila A Barskiy
  • Dmitry Budker
DOI
10.1002/mrc.5161
eISSN
1097-458X
ISSN
0749-1581
Ausgabe der Veröffentlichung
12
Zeitschrift
Magnetic Resonance in Chemistry
Sprache
en
Online publication date
2021
Paginierung
1208 - 1215
Datum der Veröffentlichung
2021
Status
Published
Herausgeber
Wiley
Herausgeber URL
http://dx.doi.org/10.1002/mrc.5161
Datum der Datenerfassung
2023
Titel
Towards large‐scale steady‐state enhanced nuclear magnetization with in situ detection
Ausgabe der Zeitschrift
59

Datenquelle: Crossref

Abstract
Signal amplification by reversible exchange (SABRE) boosts NMR signals of various nuclei enabling new applications spanning from magnetic resonance imaging to analytical chemistry and fundamental physics. SABRE is especially well positioned for continuous generation of enhanced magnetization on a large scale; however, several challenges need to be addressed for accomplishing this goal. Specifically, SABRE requires (i) a specialized catalyst capable of reversible H<sub>2</sub> activation and (ii) physical transfer of the sample from the point of magnetization generation to the point of detection (e.g., a high-field or a benchtop nuclear magnetic resonance [NMR] spectrometer). Moreover, (iii) continuous parahydrogen bubbling accelerates solvent (e.g., methanol) evaporation, thereby limiting the experimental window to tens of minutes per sample. In this work, we demonstrate a strategy to rapidly generate the best-to-date precatalyst (a compound that is chemically modified in the course of the reaction to yield the catalyst) for SABRE, [Ir(IMes)(COD)Cl] (IMes = 1,3-bis-[2,4,6-trimethylphenyl]-imidazol-2-ylidene; COD = cyclooctadiene) via a highly accessible synthesis. Second, we measure hyperpolarized samples using a home-built zero-field NMR spectrometer and study the field dependence of hyperpolarization directly in the detection apparatus, eliminating the need to physically move the sample during the experiment. Finally, we prolong the measurement time and reduce evaporation by presaturating parahydrogen with the solvent vapor before bubbling into the sample. These advancements extend opportunities for exploring SABRE hyperpolarization by researchers from various fields and pave the way to producing large quantities of hyperpolarized material for long-lasting detection of SABRE-derived nuclear magnetization.
Addresses
  • Helmholtz Institute Mainz, GSI Helmholtz Center for Heavy Ion Research GmbH, Mainz, Germany.
Autoren
  • John W Blanchard
  • Barbara Ripka
  • Benjamin A Suslick
  • Dario Gelevski
  • Teng Wu
  • Kerstin Münnemann
  • Danila A Barskiy
  • Dmitry Budker
DOI
10.1002/mrc.5161
eISSN
1097-458X
Externe Identifier
  • PubMed Identifier: 33826170
Funding acknowledgements
  • European Research Council: 695405
  • Deutsche Forschungsgemeinschaft:
  • Heising-Simons and Simons Foundations:
  • Johannes Gutenberg Universitaet Mainz:
  • Alexander von Humboldt-Stiftung:
  • Alexander von Humboldt Foundation:
  • DFG Koselleck Program:
  • Heising-Simons Foundation:
Open access
false
ISSN
0749-1581
Ausgabe der Veröffentlichung
12
Zeitschrift
Magnetic resonance in chemistry : MRC
Schlüsselwörter
  • Magnetic Resonance Imaging
  • Magnetic Resonance Spectroscopy
  • Catalysis
Sprache
eng
Medium
Print-Electronic
Online publication date
2021
Paginierung
1208 - 1215
Datum der Veröffentlichung
2021
Status
Published
Publisher licence
CC BY-NC
Datum der Datenerfassung
2021
Titel
Towards large-scale steady-state enhanced nuclear magnetization with in situ detection.
Sub types
  • Research Support, Non-U.S. Gov't
  • Journal Article
Ausgabe der Zeitschrift
59

Datenquelle: Europe PubMed Central

Abstract
Signal amplification by reversible exchange (SABRE) boosts NMR signals of various nuclei enabling new applications spanning from magnetic resonance imaging to analytical chemistry and fundamental physics. SABRE is especially well positioned for continuous generation of enhanced magnetization on a large scale; however, several challenges need to be addressed for accomplishing this goal. Specifically, SABRE requires (i) a specialized catalyst capable of reversible H2 activation and (ii) physical transfer of the sample from the point of magnetization generation to the point of detection (e.g., a high-field or a benchtop nuclear magnetic resonance [NMR] spectrometer). Moreover, (iii) continuous parahydrogen bubbling accelerates solvent (e.g., methanol) evaporation, thereby limiting the experimental window to tens of minutes per sample. In this work, we demonstrate a strategy to rapidly generate the best-to-date precatalyst (a compound that is chemically modified in the course of the reaction to yield the catalyst) for SABRE, [Ir(IMes)(COD)Cl] (IMes = 1,3-bis-[2,4,6-trimethylphenyl]-imidazol-2-ylidene; COD = cyclooctadiene) via a highly accessible synthesis. Second, we measure hyperpolarized samples using a home-built zero-field NMR spectrometer and study the field dependence of hyperpolarization directly in the detection apparatus, eliminating the need to physically move the sample during the experiment. Finally, we prolong the measurement time and reduce evaporation by presaturating parahydrogen with the solvent vapor before bubbling into the sample. These advancements extend opportunities for exploring SABRE hyperpolarization by researchers from various fields and pave the way to producing large quantities of hyperpolarized material for long-lasting detection of SABRE-derived nuclear magnetization.
Date of acceptance
2021
Autoren
  • John W Blanchard
  • Barbara Ripka
  • Benjamin A Suslick
  • Dario Gelevski
  • Teng Wu
  • Kerstin Münnemann
  • Danila A Barskiy
  • Dmitry Budker
Autoren-URL
https://www.ncbi.nlm.nih.gov/pubmed/33826170
DOI
10.1002/mrc.5161
eISSN
1097-458X
Funding acknowledgements
  • Deutsche Forschungsgemeinschaft:
  • Heising-Simons Foundation:
  • DFG Koselleck Program:
  • Heising-Simons and Simons Foundations:
  • Alexander von Humboldt Foundation:
  • Johannes Gutenberg Universitaet Mainz:
  • European Research Council: 695405
Ausgabe der Veröffentlichung
12
Zeitschrift
Magn Reson Chem
Schlüsselwörter
  • PHIP
  • SABRE
  • hyperpolarization
  • in situ detection
  • parahydrogen
  • Catalysis
  • Magnetic Resonance Imaging
  • Magnetic Resonance Spectroscopy
Sprache
eng
Country
England
Paginierung
1208 - 1215
Datum der Veröffentlichung
2021
Status
Published
Datum, an dem der Datensatz öffentlich gemacht wurde
2022
Titel
Towards large-scale steady-state enhanced nuclear magnetization with in situ detection.
Sub types
  • Journal Article
  • Research Support, Non-U.S. Gov't
Ausgabe der Zeitschrift
59

Datenquelle: PubMed

Author's licence
CC-BY-NC
Autoren
  • John W Blanchard
  • Barbara Ripka
  • Benjamin A Suslick
  • Dario Gelevski
  • Teng Wu
  • Kerstin Münnemann
  • Danila A Barskiy
  • Dmitry Budker
Hosting institution
Universitätsbibliothek Mainz
Sammlungen
  • JGU-Publikationen
Resource version
Published version
DOI
10.1002/mrc.5161
File(s) embargoed
false
Open access
true
ISSN
1097-458X
Ausgabe der Veröffentlichung
12
Zeitschrift
Magnetic resonance in chemistry
Schlüsselwörter
  • 530 Physik
  • 530 Physics
  • 540 Chemie
  • 540 Chemistry and allied sciences
Sprache
eng
Open access status
Open Access
Paginierung
1208 - 1215
Datum der Veröffentlichung
2021
Public URL
https://openscience.ub.uni-mainz.de/handle/20.500.12030/8102
Herausgeber
Wiley
Datum der Datenerfassung
2022
Datum, an dem der Datensatz öffentlich gemacht wurde
2022
Zugang
Public
Titel
Towards large-scale steady-state enhanced nuclear magnetization with in situ detection
Ausgabe der Zeitschrift
59

Files

towards_largescale_steadystat-20221017155708364.pdf

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