Effects of biradical deuteration on the performance of DNP: Towards better performing polarizing agents

Perras, Frédéric A.; Reinig, Regina R.; Slowing, Igor I.; Sadow, Aaron D.; Pruski, Marek

doi:10.1039/C5CP06505D

Title: Effects of biradical deuteration on the performance of DNP: Towards better performing polarizing agents

Journal Article · Fri Nov 20 00:00:00 EST 2015 · Physical Chemistry Chemical Physics. PCCP

DOI:https://doi.org/10.1039/C5CP06505D· OSTI ID:1227445

Perras, Frédéric A. ^[1]; Reinig, Regina R. ^[2]; Slowing, Igor I. ^[2]; Sadow, Aaron D. ^[2]; Pruski, Marek ^[2]

Ames Lab., Ames, IA (United States)
Ames Lab., Ames, IA (United States); Iowa State Univ., Ames, IA (United States)

We study the effects of the deuteration of biradical polarizing agents on the efficiency of dynamic nuclear polarization (DNP) via the cross-effect. To this end, we synthesized a series of bTbK and TOTAPol biradicals with systematically increased deuterium substitution. The deuteration increases the radicals' relaxation time, thus contributing to a higher saturation factor and larger DNP enhancement, and reduces the pool of protons within the so-called spin diffusion barrier. Notably, we report that full or partial deuteration leads to improved DNP enhancement factors in standard samples, but also slows down the build-up of hyperpolarization. Improvements in DNP enhancements factors of up to 70% and time savings of up to 38% are obtained upon full deuteration. As a result, it is foreseen that this approach may be applied to other DNP polarizing agents thus enabling further sensitivity improvements.

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Research Organization:: Ames Lab., Ames, IA (United States)

Sponsoring Organization:: USDOE

Grant/Contract Number:: AC02-07CH11358

OSTI ID:: 1227445

Report Number(s):: IS-J-8842; PPCPFQ

Journal Information:: Physical Chemistry Chemical Physics. PCCP, Vol. 18, Issue 1; ISSN 1463-9076

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 26 works

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Efficiency of Water-Soluble Nitroxide Biradicals for Dynamic Nuclear Polarization in Rotating Solids at 9.4 T: bcTol-M and cyolyl-TOTAPOL as New Polarizing Agents Geiger, Michel-Andreas; Jagtap, Anil P.; Kaushik, Monu Chemistry - A European Journal, Vol. 24, Issue 51 https://doi.org/10.1002/chem.201801251	journal	August 2018
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Optimizing nitroxide biradicals for cross-effect MAS-DNP: the role of g -tensors’ distance Mentink-Vigier, Frédéric Physical Chemistry Chemical Physics, Vol. 22, Issue 6 https://doi.org/10.1039/c9cp06201g	journal	January 2020
First α-deuterium nitroxides; synthesis and EPR study Toledo, Hila; Tumanskii, Boris; Sabirov, Denis Sh. Organic & Biomolecular Chemistry, Vol. 17, Issue 34 https://doi.org/10.1039/c9ob01127g	journal	January 2019
Large-scale ab initio simulations of MAS DNP enhancements using a Monte Carlo optimization strategy Perras, Frédéric A.; Pruski, Marek The Journal of Chemical Physics, Vol. 149, Issue 15 https://doi.org/10.1063/1.5042651	journal	October 2018
¹⁹ F Magic Angle Spinning Dynamic Nuclear Polarization Enhanced NMR Spectroscopy Viger‐Gravel, Jasmine; Avalos, Claudia E.; Kubicki, Dominik J. Angewandte Chemie International Edition, Vol. 58, Issue 22 https://doi.org/10.1002/anie.201814416	journal	May 2019

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