Molecular sensing with hyperpolarized 129Xe using switchable chemical exchange relaxation transfer

A new approach for hyperpolarized 129Xe molecular sensors is explored using paramagnetic relaxation agents that can be deactivated upon chemical or enzymatic reaction with an analyte. Cryptophane encapsulated 129Xe within the vicinity of the paramagnetic center experiences fast relaxation that, thro...

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Main Authors: Zamberlan, Francesco, Lesbats, Clémentine, Rogers, Nicola J., Krupa, James L., Pavlovskaya, Galina E., Thomas, Neil R., Faas, Henryk, Meersmann, Thomas
Format: Article
Published: Wiley-VCH 2015
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Online Access:https://eprints.nottingham.ac.uk/31550/
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author Zamberlan, Francesco
Lesbats, Clémentine
Rogers, Nicola J.
Krupa, James L.
Pavlovskaya, Galina E.
Thomas, Neil R.
Faas, Henryk
Meersmann, Thomas
author_facet Zamberlan, Francesco
Lesbats, Clémentine
Rogers, Nicola J.
Krupa, James L.
Pavlovskaya, Galina E.
Thomas, Neil R.
Faas, Henryk
Meersmann, Thomas
author_sort Zamberlan, Francesco
building Nottingham Research Data Repository
collection Online Access
description A new approach for hyperpolarized 129Xe molecular sensors is explored using paramagnetic relaxation agents that can be deactivated upon chemical or enzymatic reaction with an analyte. Cryptophane encapsulated 129Xe within the vicinity of the paramagnetic center experiences fast relaxation that, through chemical exchange of xenon atoms between cage and solvent pool, causes accelerated hyperpolarized 129Xe signal decay in the dissolved phase. In this work, the relaxivity of GadoliniumIII-DOTA on 129Xe in the solvent was increased eightfold through tethering of the paramagnetic molecule to a cryptophane cage. This potent relaxation agent can be ‘turned off’ specifically for 129Xe through chemical reactions that spatially separate the GdIII centre from the attached cryptophane cage. Unlike 129Xe chemical shift based sensors, the new concept does not require high spectral resolution and may lead to a new generation of responsive contrast agents for molecular MRI.
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spelling nottingham-315502020-05-04T17:15:48Z https://eprints.nottingham.ac.uk/31550/ Molecular sensing with hyperpolarized 129Xe using switchable chemical exchange relaxation transfer Zamberlan, Francesco Lesbats, Clémentine Rogers, Nicola J. Krupa, James L. Pavlovskaya, Galina E. Thomas, Neil R. Faas, Henryk Meersmann, Thomas A new approach for hyperpolarized 129Xe molecular sensors is explored using paramagnetic relaxation agents that can be deactivated upon chemical or enzymatic reaction with an analyte. Cryptophane encapsulated 129Xe within the vicinity of the paramagnetic center experiences fast relaxation that, through chemical exchange of xenon atoms between cage and solvent pool, causes accelerated hyperpolarized 129Xe signal decay in the dissolved phase. In this work, the relaxivity of GadoliniumIII-DOTA on 129Xe in the solvent was increased eightfold through tethering of the paramagnetic molecule to a cryptophane cage. This potent relaxation agent can be ‘turned off’ specifically for 129Xe through chemical reactions that spatially separate the GdIII centre from the attached cryptophane cage. Unlike 129Xe chemical shift based sensors, the new concept does not require high spectral resolution and may lead to a new generation of responsive contrast agents for molecular MRI. Wiley-VCH 2015-08-03 Article PeerReviewed Zamberlan, Francesco, Lesbats, Clémentine, Rogers, Nicola J., Krupa, James L., Pavlovskaya, Galina E., Thomas, Neil R., Faas, Henryk and Meersmann, Thomas (2015) Molecular sensing with hyperpolarized 129Xe using switchable chemical exchange relaxation transfer. ChemPhysChem, 16 (11). pp. 2294-2298. ISSN 1439-7641 Hyperpolarized xenon biosensor • MRI contrast agent • cryptophane • HyperCEST • molecular imaging http://onlinelibrary.wiley.com/doi/10.1002/cphc.201500367/abstract doi:10.1002/cphc.201500367 doi:10.1002/cphc.201500367
spellingShingle Hyperpolarized xenon biosensor • MRI contrast agent • cryptophane • HyperCEST • molecular imaging
Zamberlan, Francesco
Lesbats, Clémentine
Rogers, Nicola J.
Krupa, James L.
Pavlovskaya, Galina E.
Thomas, Neil R.
Faas, Henryk
Meersmann, Thomas
Molecular sensing with hyperpolarized 129Xe using switchable chemical exchange relaxation transfer
title Molecular sensing with hyperpolarized 129Xe using switchable chemical exchange relaxation transfer
title_full Molecular sensing with hyperpolarized 129Xe using switchable chemical exchange relaxation transfer
title_fullStr Molecular sensing with hyperpolarized 129Xe using switchable chemical exchange relaxation transfer
title_full_unstemmed Molecular sensing with hyperpolarized 129Xe using switchable chemical exchange relaxation transfer
title_short Molecular sensing with hyperpolarized 129Xe using switchable chemical exchange relaxation transfer
title_sort molecular sensing with hyperpolarized 129xe using switchable chemical exchange relaxation transfer
topic Hyperpolarized xenon biosensor • MRI contrast agent • cryptophane • HyperCEST • molecular imaging
url https://eprints.nottingham.ac.uk/31550/
https://eprints.nottingham.ac.uk/31550/
https://eprints.nottingham.ac.uk/31550/