Skip to main content
  • Submit
  • About
    • Editorial Board
    • PNAS Staff
    • FAQ
    • Accessibility Statement
    • Rights and Permissions
    • Site Map
  • Contact
  • Journal Club
  • Subscribe
    • Subscription Rates
    • Subscriptions FAQ
    • Open Access
    • Recommend PNAS to Your Librarian
  • Log in
  • My Cart

Main menu

  • Home
  • Articles
    • Current
    • Special Feature Articles - Most Recent
    • Special Features
    • Colloquia
    • Collected Articles
    • PNAS Classics
    • List of Issues
  • Front Matter
  • News
    • For the Press
    • This Week In PNAS
    • PNAS in the News
  • Podcasts
  • Authors
    • Information for Authors
    • Editorial and Journal Policies
    • Submission Procedures
    • Fees and Licenses
  • Submit
  • About
    • Editorial Board
    • PNAS Staff
    • FAQ
    • Accessibility Statement
    • Rights and Permissions
    • Site Map
  • Contact
  • Journal Club
  • Subscribe
    • Subscription Rates
    • Subscriptions FAQ
    • Open Access
    • Recommend PNAS to Your Librarian

User menu

  • Log in
  • My Cart

Search

  • Advanced search
Home
Home

Advanced Search

  • Home
  • Articles
    • Current
    • Special Feature Articles - Most Recent
    • Special Features
    • Colloquia
    • Collected Articles
    • PNAS Classics
    • List of Issues
  • Front Matter
  • News
    • For the Press
    • This Week In PNAS
    • PNAS in the News
  • Podcasts
  • Authors
    • Information for Authors
    • Editorial and Journal Policies
    • Submission Procedures
    • Fees and Licenses

New Research In

Physical Sciences

Featured Portals

  • Physics
  • Chemistry
  • Sustainability Science

Articles by Topic

  • Applied Mathematics
  • Applied Physical Sciences
  • Astronomy
  • Computer Sciences
  • Earth, Atmospheric, and Planetary Sciences
  • Engineering
  • Environmental Sciences
  • Mathematics
  • Statistics

Social Sciences

Featured Portals

  • Anthropology
  • Sustainability Science

Articles by Topic

  • Economic Sciences
  • Environmental Sciences
  • Political Sciences
  • Psychological and Cognitive Sciences
  • Social Sciences

Biological Sciences

Featured Portals

  • Sustainability Science

Articles by Topic

  • Agricultural Sciences
  • Anthropology
  • Applied Biological Sciences
  • Biochemistry
  • Biophysics and Computational Biology
  • Cell Biology
  • Developmental Biology
  • Ecology
  • Environmental Sciences
  • Evolution
  • Genetics
  • Immunology and Inflammation
  • Medical Sciences
  • Microbiology
  • Neuroscience
  • Pharmacology
  • Physiology
  • Plant Biology
  • Population Biology
  • Psychological and Cognitive Sciences
  • Sustainability Science
  • Systems Biology
Research Article

Hybrid polarizing solids for pure hyperpolarized liquids through dissolution dynamic nuclear polarization

David Gajan, Aurélien Bornet, Basile Vuichoud, Jonas Milani, Roberto Melzi, Henri A. van Kalkeren, Laurent Veyre, Chloé Thieuleux, Matthew P. Conley, Wolfram R. Grüning, Martin Schwarzwälder, Anne Lesage, Christophe Copéret, Geoffrey Bodenhausen, Lyndon Emsley, and Sami Jannin
PNAS October 14, 2014 111 (41) 14693-14697; first published September 29, 2014; https://doi.org/10.1073/pnas.1407730111
David Gajan
aCentre de Résonance Magnétique Nucléaire (RMN) à Très Hauts Champs, Institut des Sciences Analytiques [Centre National de la Recherche Scientifique (CNRS)/Ecole Normale Supérieure (ENS) Lyon/Université Claude Bernard Lyon 1 (UCBL)], Université de Lyon, 69100 Villeurbanne, France;
  • Find this author on Google Scholar
  • Find this author on PubMed
  • Search for this author on this site
Aurélien Bornet
bInstitut des Sciences et Ingénierie Chimiques, Ecole Polytechnique Fédérale de Lausanne (EPFL), CH-1015 Lausanne, Switzerland;
  • Find this author on Google Scholar
  • Find this author on PubMed
  • Search for this author on this site
Basile Vuichoud
bInstitut des Sciences et Ingénierie Chimiques, Ecole Polytechnique Fédérale de Lausanne (EPFL), CH-1015 Lausanne, Switzerland;
  • Find this author on Google Scholar
  • Find this author on PubMed
  • Search for this author on this site
Jonas Milani
bInstitut des Sciences et Ingénierie Chimiques, Ecole Polytechnique Fédérale de Lausanne (EPFL), CH-1015 Lausanne, Switzerland;
  • Find this author on Google Scholar
  • Find this author on PubMed
  • Search for this author on this site
Roberto Melzi
cBruker Italia S.r.l., IT-20158 Milan, Italy;
  • Find this author on Google Scholar
  • Find this author on PubMed
  • Search for this author on this site
Henri A. van Kalkeren
dUniversité de Lyon, Institut de Chimie de Lyon, Laboratoire de Chimie, Catalyse, Polymères et Procédés (LC2P2), Unité Mixte de Recherche (UMR) 5265 Centre National de la Recherche Scientifique (CNRS)-Ecole Supérieure de Chimie Physique Electronique de Lyon (CPE Lyon)-Université Claude Bernard Lyon 1 (UCBL), Ecole Supérieure de Chimie Physique Electronique de Lyon (CPE Lyon), 69100 Villeurbanne, France;
  • Find this author on Google Scholar
  • Find this author on PubMed
  • Search for this author on this site
Laurent Veyre
dUniversité de Lyon, Institut de Chimie de Lyon, Laboratoire de Chimie, Catalyse, Polymères et Procédés (LC2P2), Unité Mixte de Recherche (UMR) 5265 Centre National de la Recherche Scientifique (CNRS)-Ecole Supérieure de Chimie Physique Electronique de Lyon (CPE Lyon)-Université Claude Bernard Lyon 1 (UCBL), Ecole Supérieure de Chimie Physique Electronique de Lyon (CPE Lyon), 69100 Villeurbanne, France;
  • Find this author on Google Scholar
  • Find this author on PubMed
  • Search for this author on this site
Chloé Thieuleux
dUniversité de Lyon, Institut de Chimie de Lyon, Laboratoire de Chimie, Catalyse, Polymères et Procédés (LC2P2), Unité Mixte de Recherche (UMR) 5265 Centre National de la Recherche Scientifique (CNRS)-Ecole Supérieure de Chimie Physique Electronique de Lyon (CPE Lyon)-Université Claude Bernard Lyon 1 (UCBL), Ecole Supérieure de Chimie Physique Electronique de Lyon (CPE Lyon), 69100 Villeurbanne, France;
  • Find this author on Google Scholar
  • Find this author on PubMed
  • Search for this author on this site
Matthew P. Conley
eDepartment of Chemistry and Applied Biosciences, Eidgenössiche Technische Hochschule (ETH), 8093 Zurich, Switzerland;
  • Find this author on Google Scholar
  • Find this author on PubMed
  • Search for this author on this site
Wolfram R. Grüning
eDepartment of Chemistry and Applied Biosciences, Eidgenössiche Technische Hochschule (ETH), 8093 Zurich, Switzerland;
  • Find this author on Google Scholar
  • Find this author on PubMed
  • Search for this author on this site
Martin Schwarzwälder
eDepartment of Chemistry and Applied Biosciences, Eidgenössiche Technische Hochschule (ETH), 8093 Zurich, Switzerland;
  • Find this author on Google Scholar
  • Find this author on PubMed
  • Search for this author on this site
Anne Lesage
aCentre de Résonance Magnétique Nucléaire (RMN) à Très Hauts Champs, Institut des Sciences Analytiques [Centre National de la Recherche Scientifique (CNRS)/Ecole Normale Supérieure (ENS) Lyon/Université Claude Bernard Lyon 1 (UCBL)], Université de Lyon, 69100 Villeurbanne, France;
  • Find this author on Google Scholar
  • Find this author on PubMed
  • Search for this author on this site
Christophe Copéret
eDepartment of Chemistry and Applied Biosciences, Eidgenössiche Technische Hochschule (ETH), 8093 Zurich, Switzerland;
  • Find this author on Google Scholar
  • Find this author on PubMed
  • Search for this author on this site
Geoffrey Bodenhausen
bInstitut des Sciences et Ingénierie Chimiques, Ecole Polytechnique Fédérale de Lausanne (EPFL), CH-1015 Lausanne, Switzerland;
fDépartement de Chimie, Ecole Normale Supérieure (ENS)-Paris Sciences et Lettres (PSL) Research University, F-75005 Paris, France;
gLaboratoire de Biomolécules (LBM), Université Pierre et Marie Curie (UPMC) Université Paris 06, Sorbonnes Universités, F-75005 Paris, France; and
hLaboratoire de Biomolécules (LBM), Unité Mixte de Recherche (UMR) 7203 Centre National de la Recherche Scientifique (CNRS), F-75005 Paris, France
  • Find this author on Google Scholar
  • Find this author on PubMed
  • Search for this author on this site
Lyndon Emsley
aCentre de Résonance Magnétique Nucléaire (RMN) à Très Hauts Champs, Institut des Sciences Analytiques [Centre National de la Recherche Scientifique (CNRS)/Ecole Normale Supérieure (ENS) Lyon/Université Claude Bernard Lyon 1 (UCBL)], Université de Lyon, 69100 Villeurbanne, France;
bInstitut des Sciences et Ingénierie Chimiques, Ecole Polytechnique Fédérale de Lausanne (EPFL), CH-1015 Lausanne, Switzerland;
  • Find this author on Google Scholar
  • Find this author on PubMed
  • Search for this author on this site
  • For correspondence: lyndon.emsley@ens-lyon.fr
Sami Jannin
bInstitut des Sciences et Ingénierie Chimiques, Ecole Polytechnique Fédérale de Lausanne (EPFL), CH-1015 Lausanne, Switzerland;
  • Find this author on Google Scholar
  • Find this author on PubMed
  • Search for this author on this site
  1. Edited* by Timothy M. Swager, Massachusetts Institute of Technology, Cambridge, MA, and approved August 25, 2014 (received for review April 30, 2014)

  • Article
  • Figures & SI
  • Info & Metrics
  • PDF
Loading

Significance

Hyperpolarization by dissolution dynamic nuclear polarization can dramatically enhance signal intensities in MRI and NMR, notably for metabolic tracers for imaging and diagnosis. It is applicable to a variety of substrates for in vivo imaging and chemistry but requires the use of contaminants (glassing agents and free radicals) that may interact with cells and proteins and can have potential side effects. These contaminants can sometimes be eliminated by precipitation followed by filtration or solvent extraction, but these methods are substrate-specific, are usually time-consuming, and typically result in signal loss. Here, production of pure hyperpolarized liquids free of contaminants is shown by a simple wetting–polarization–filtration sequence for a solid silica matrix containing homogeneously distributed persistent radicals.

Abstract

Hyperpolarization of substrates for magnetic resonance spectroscopy (MRS) and imaging (MRI) by dissolution dynamic nuclear polarization (D-DNP) usually involves saturating the ESR transitions of polarizing agents (PAs; e.g., persistent radicals embedded in frozen glassy matrices). This approach has shown enormous potential to achieve greatly enhanced nuclear spin polarization, but the presence of PAs and/or glassing agents in the sample after dissolution can raise concerns for in vivo MRI applications, such as perturbing molecular interactions, and may induce the erosion of hyperpolarization in spectroscopy and MRI. We show that D-DNP can be performed efficiently with hybrid polarizing solids (HYPSOs) with 2,2,6,6-tetramethyl-piperidine-1-oxyl radicals incorporated in a mesostructured silica material and homogeneously distributed along its pore channels. The powder is wetted with a solution containing molecules of interest (for example, metabolites for MRS or MRI) to fill the pore channels (incipient wetness impregnation), and DNP is performed at low temperatures in a very efficient manner. This approach allows high polarization without the need for glass-forming agents and is applicable to a broad range of substrates, including peptides and metabolites. During dissolution, HYPSO is physically retained by simple filtration in the cryostat of the DNP polarizer, and a pure hyperpolarized solution is collected within a few seconds. The resulting solution contains the pure substrate, is free from any paramagnetic or other pollutants, and is ready for in vivo infusion.

  • D-DNP
  • NMR signal enhancement
  • molecular imaging
  • mesostructured hybrid silica
  • porous materials

Footnotes

  • ↵1To whom correspondence should be addressed. Email: lyndon.emsley{at}ens-lyon.fr.
  • Author contributions: D.G., A.L., C.C., G.B., L.E., and S.J. designed research; D.G., A.B., B.V., J.M., H.A.v.K., L.V., M.P.C., W.R.G., M.S., and S.J. performed research; H.A.v.K., M.P.C., W.R.G., and M.S. contributed new reagents/analytic tools; D.G., A.B., B.V., J.M., R.M., C.T., A.L., C.C., G.B., L.E., and S.J. analyzed data; and D.G., C.T., C.C., G.B., L.E., and S.J. wrote the paper.

  • The authors declare no conflict of interest.

  • ↵*This Direct Submission article had a prearranged editor.

  • This article contains supporting information online at www.pnas.org/lookup/suppl/doi:10.1073/pnas.1407730111/-/DCSupplemental.

Freely available online through the PNAS open access option.

View Full Text
PreviousNext
Back to top
Article Alerts
Email Article

Thank you for your interest in spreading the word on PNAS.

NOTE: We only request your email address so that the person you are recommending the page to knows that you wanted them to see it, and that it is not junk mail. We do not capture any email address.

Enter multiple addresses on separate lines or separate them with commas.
Hybrid polarizing solids for pure hyperpolarized liquids through dissolution dynamic nuclear polarization
(Your Name) has sent you a message from PNAS
(Your Name) thought you would like to see the PNAS web site.
CAPTCHA
This question is for testing whether or not you are a human visitor and to prevent automated spam submissions.
Citation Tools
Hybrid solids for pure hyperpolarized liquids
David Gajan, Aurélien Bornet, Basile Vuichoud, Jonas Milani, Roberto Melzi, Henri A. van Kalkeren, Laurent Veyre, Chloé Thieuleux, Matthew P. Conley, Wolfram R. Grüning, Martin Schwarzwälder, Anne Lesage, Christophe Copéret, Geoffrey Bodenhausen, Lyndon Emsley, Sami Jannin
Proceedings of the National Academy of Sciences Oct 2014, 111 (41) 14693-14697; DOI: 10.1073/pnas.1407730111

Citation Manager Formats

  • BibTeX
  • Bookends
  • EasyBib
  • EndNote (tagged)
  • EndNote 8 (xml)
  • Medlars
  • Mendeley
  • Papers
  • RefWorks Tagged
  • Ref Manager
  • RIS
  • Zotero
Request Permissions
Share
Hybrid solids for pure hyperpolarized liquids
David Gajan, Aurélien Bornet, Basile Vuichoud, Jonas Milani, Roberto Melzi, Henri A. van Kalkeren, Laurent Veyre, Chloé Thieuleux, Matthew P. Conley, Wolfram R. Grüning, Martin Schwarzwälder, Anne Lesage, Christophe Copéret, Geoffrey Bodenhausen, Lyndon Emsley, Sami Jannin
Proceedings of the National Academy of Sciences Oct 2014, 111 (41) 14693-14697; DOI: 10.1073/pnas.1407730111
Digg logo Reddit logo Twitter logo Facebook logo Google logo Mendeley logo
  • Tweet Widget
  • Facebook Like
  • Mendeley logo Mendeley
Proceedings of the National Academy of Sciences: 111 (41)
Table of Contents

Submit

Sign up for Article Alerts

Article Classifications

  • Physical Sciences
  • Chemistry

Jump to section

  • Article
    • Abstract
    • Results and Discussion
    • Methods
    • Acknowledgments
    • Footnotes
    • References
  • Figures & SI
  • Info & Metrics
  • PDF

You May Also be Interested in

Abstract depiction of a guitar and musical note
Science & Culture: At the nexus of music and medicine, some see disease treatments
Although the evidence is still limited, a growing body of research suggests music may have beneficial effects for diseases such as Parkinson’s.
Image credit: Shutterstock/agsandrew.
Large piece of gold
News Feature: Tracing gold's cosmic origins
Astronomers thought they’d finally figured out where gold and other heavy elements in the universe came from. In light of recent results, they’re not so sure.
Image credit: Science Source/Tom McHugh.
Dancers in red dresses
Journal Club: Friends appear to share patterns of brain activity
Researchers are still trying to understand what causes this strong correlation between neural and social networks.
Image credit: Shutterstock/Yeongsik Im.
White and blue bird
Hazards of ozone pollution to birds
Amanda Rodewald, Ivan Rudik, and Catherine Kling talk about the hazards of ozone pollution to birds.
Listen
Past PodcastsSubscribe
Goats standing in a pin
Transplantation of sperm-producing stem cells
CRISPR-Cas9 gene editing can improve the effectiveness of spermatogonial stem cell transplantation in mice and livestock, a study finds.
Image credit: Jon M. Oatley.

Similar Articles

Site Logo
Powered by HighWire
  • Submit Manuscript
  • Twitter
  • Facebook
  • RSS Feeds
  • Email Alerts

Articles

  • Current Issue
  • Special Feature Articles – Most Recent
  • List of Issues

PNAS Portals

  • Anthropology
  • Chemistry
  • Classics
  • Front Matter
  • Physics
  • Sustainability Science
  • Teaching Resources

Information

  • Authors
  • Editorial Board
  • Reviewers
  • Librarians
  • Press
  • Site Map
  • PNAS Updates

Feedback    Privacy/Legal

Copyright © 2021 National Academy of Sciences. Online ISSN 1091-6490