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research article

Electrochemical Overhauser dynamic nuclear polarization

Tamski, Mika  
•
Milani, Jonas  
•
Roussel, Christophe  
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August 28, 2020
Physical Chemistry Chemical Physics

Nuclear Magnetic Resonance (NMR) spectroscopy suffers from low sensitivity due to the low nuclear spin polarization obtained within practically achievable external magnetic fields. Dynamic Nuclear Polarization (DNP) refers to techniques that increase the NMR signal intensity by transferring spin polarization from electrons to the nuclei. Until now, a common method of introducing unpaired electrons to a sample has been to add to it a radical such as TEMPOL or trityl. The alternative we address here is to use electrochemical oxidation and/or reduction of a redox mediator to generate radical species that can be used for DNP. Surprisingly, the potential of electrochemically-generated radicals as a source of hyperpolarization for DNP has not been investigated so far. In this communication, we show the proof of principle of performing anin situDNP experiment at a low magnetic field in a solution phase, with electrochemically generated methyl viologen cation radicals. Electrochemistry as a source of radicals can offer exciting prospects for DNP. The electrode may be one that generates radicals with a high spin polarization. The concentration of radicals in the sample can be adjusted by changing the duration and magnitude of the applied electrode potential. Removal of the radical from the sample after spin polarization transfer is also possible, thereby increasing the lifetime of the nuclear hyperpolarization.

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Type
research article
DOI
10.1039/d0cp00984a
Web of Science ID

WOS:000562560400001

Author(s)
Tamski, Mika  
Milani, Jonas  
Roussel, Christophe  
Ansermet, Jean-Philippe  
Date Issued

2020-08-28

Published in
Physical Chemistry Chemical Physics
Volume

22

Issue

32

Start page

17769

End page

17776

Subjects

Chemistry, Physical

•

Physics, Atomic, Molecular & Chemical

•

Chemistry

•

Physics

•

electron-spin-resonance

•

liquid-state dnp

•

magnetic-resonance

•

hydration dynamics

•

nmr spectroelectrochemistry

•

free-radicals

•

enhancement

•

product

Note

This article is licensed under a Creative Commons Attribution 3.0 Unported Licence.

Editorial or Peer reviewed

REVIEWED

Written at

EPFL

EPFL units
LPMN  
SB-SCGC  
Available on Infoscience
September 10, 2020
Use this identifier to reference this record
https://infoscience.epfl.ch/handle/20.500.14299/171522
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