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Direct production of a hyperpolarized metabolite on a microfluidic chip

Direct production of a hyperpolarized metabolite on a microfluidic chip
Direct production of a hyperpolarized metabolite on a microfluidic chip
Microfluidic systems hold great potential for the study of live microscopic cultures of cells, tissue samples, and small organisms. Integration of hyperpolarization would enable quantitative studies of metabolism in such volume limited systems by high-resolution NMR spectroscopy. We demonstrate, for the first time, the integrated generation and detection of a hyperpolarized metabolite on a microfluidic chip. The metabolite [1-13C]fumarate is produced in a nuclear hyperpolarized form by (i) introducing para-enriched hydrogen into the solution by diffusion through a polymer membrane, (ii) reaction with a substrate in the presence of a ruthenium-based catalyst, and (iii) conversion of the singlet-polarized reaction product into a magnetized form by the application of a radiofrequency pulse sequence, all on the same microfluidic chip. The microfluidic device delivers a continuous flow of hyperpolarized material at the 2.5 μL/min scale, with a polarization level of 4%. We demonstrate two methods for mitigating singlet–triplet mixing effects which otherwise reduce the achieved polarization level.
0003-2700
3260-3267
Barker, Sylwia, Joanna
868bcd37-9c33-4b12-983c-3d2d2909b94a
Dagys, Laurynas
0de61597-b152-4bee-a934-123a9d2de883
Hale, William G
d98f9d64-00f9-447e-9783-185185a0b3c6
Ripka, Barbara H
4eaf858c-09a2-4072-97d0-912585c371cd
Eills, James
23130b21-68fa-4c8b-9399-e55f2e71ef36
Sharma, Manvendra
e249236d-221d-4e59-8440-011f6863f891
Levitt, Malcolm H.
bcc5a80a-e5c5-4e0e-9a9a-249d036747c3
Utz, Marcel
c84ed64c-9e89-4051-af39-d401e423891b
Barker, Sylwia, Joanna
868bcd37-9c33-4b12-983c-3d2d2909b94a
Dagys, Laurynas
0de61597-b152-4bee-a934-123a9d2de883
Hale, William G
d98f9d64-00f9-447e-9783-185185a0b3c6
Ripka, Barbara H
4eaf858c-09a2-4072-97d0-912585c371cd
Eills, James
23130b21-68fa-4c8b-9399-e55f2e71ef36
Sharma, Manvendra
e249236d-221d-4e59-8440-011f6863f891
Levitt, Malcolm H.
bcc5a80a-e5c5-4e0e-9a9a-249d036747c3
Utz, Marcel
c84ed64c-9e89-4051-af39-d401e423891b

Barker, Sylwia, Joanna, Dagys, Laurynas, Hale, William G, Ripka, Barbara H, Eills, James, Sharma, Manvendra, Levitt, Malcolm H. and Utz, Marcel (2022) Direct production of a hyperpolarized metabolite on a microfluidic chip. Analytical Chemistry, 94 (7), 3260-3267. (doi:10.1021/acs.analchem.1c05030).

Record type: Article

Abstract

Microfluidic systems hold great potential for the study of live microscopic cultures of cells, tissue samples, and small organisms. Integration of hyperpolarization would enable quantitative studies of metabolism in such volume limited systems by high-resolution NMR spectroscopy. We demonstrate, for the first time, the integrated generation and detection of a hyperpolarized metabolite on a microfluidic chip. The metabolite [1-13C]fumarate is produced in a nuclear hyperpolarized form by (i) introducing para-enriched hydrogen into the solution by diffusion through a polymer membrane, (ii) reaction with a substrate in the presence of a ruthenium-based catalyst, and (iii) conversion of the singlet-polarized reaction product into a magnetized form by the application of a radiofrequency pulse sequence, all on the same microfluidic chip. The microfluidic device delivers a continuous flow of hyperpolarized material at the 2.5 μL/min scale, with a polarization level of 4%. We demonstrate two methods for mitigating singlet–triplet mixing effects which otherwise reduce the achieved polarization level.

Text
fumarate@chip - Accepted Manuscript
Restricted to Repository staff only until 11 February 2023.
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More information

Accepted/In Press date: 24 January 2022
e-pub ahead of print date: 11 February 2022
Published date: 22 February 2022
Additional Information: The authors are indebted to Dr. Christian Bengs and Dr. Giuseppe Pileio for help with the SpinDynamica simulations, as well as for insightful discussions about the results and theory. This work has been supported by an EPSRC iCASE studentship EP/R513325/1 to SJB, co-funded by Bruker UK Ltd., as well as by the EU H2020 FETOpen Project "TISuMR" (Grant number 737043). This project has also received funding from the European Union’s Horizon 2020 research and innova�tion programme under the Marie Skłodowska-Curie Grant Agreement No. 766402, as well as ERC project 786707-FunMagResBeacons, and EPSRC grants EP/P009980/1 and EP/V055593/1.

Identifiers

Local EPrints ID: 454568
URI: http://eprints.soton.ac.uk/id/eprint/454568
ISSN: 0003-2700
PURE UUID: bef14c9e-fe1b-46cb-9a9b-08901ce6ff83
ORCID for Malcolm H. Levitt: ORCID iD orcid.org/0000-0001-9878-1180
ORCID for Marcel Utz: ORCID iD orcid.org/0000-0003-2274-9672

Catalogue record

Date deposited: 16 Feb 2022 17:37
Last modified: 03 Sep 2022 01:48

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Contributors

Author: Sylwia, Joanna Barker
Author: Laurynas Dagys
Author: William G Hale
Author: Barbara H Ripka
Author: James Eills
Author: Manvendra Sharma
Author: Marcel Utz ORCID iD

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