Effects of biradical deuteration on the performance of DNP: towards better performing polarizing agents
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...
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creator | Perras, Frédéric A Reinig, Regina R Slowing, Igor I Sadow, Aaron D Pruski, Marek |
description | 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. It is foreseen that this approach may be applied to other DNP polarizing agents thus enabling further sensitivity improvements. |
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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. 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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. It is foreseen that this approach may be applied to other DNP polarizing agents thus enabling further sensitivity improvements.</description><subject>Deuteration</subject><subject>Deuterium</subject><subject>Diffusion barriers</subject><subject>Dynamic tests</subject><subject>INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY</subject><subject>Polarization</subject><subject>Radicals</subject><subject>Saturation</subject><issn>1463-9076</issn><issn>1463-9084</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2016</creationdate><recordtype>article</recordtype><recordid>eNqF0U1LAzEQBuAgitbqxR8giycRqsluPjbepPULivag5yWbTGpku1mTFNFf79baXoXAzOFhmMyL0AnBlwQX8koz3WHOMDM7aEAoL0YSl3R32wt-gA5jfMcYE0aKfXSQc04kZmyA5rfWgk4x8zarXVDGadVkBpYJgkrOt1n_0htkHQTrw0K1GlZ28jS7zpL_VMHErIbU8w1x7TzrfKOC-161ag5tikdoz6omwvFfHaLXu9uX8cNo-nz_OL6ZjjQteRopxYUlXBLBWA2ytMqU_aKAjRJgdG0sBS5lbU2uCM0pt1IJBgaXmrE8x8UQna3n-phcFbVLoN-0b9v-kxXJc0Ep69H5GnXBfywhpmrhooamUS34ZaxISXh_wVyI_6lgmBZMyLKnF2uqg48xgK264BYqfFUEV6ugqjEbz36DmvT49G_usl6A2dJNMsUPVOCOVw</recordid><startdate>2016</startdate><enddate>2016</enddate><creator>Perras, Frédéric A</creator><creator>Reinig, Regina R</creator><creator>Slowing, Igor I</creator><creator>Sadow, Aaron D</creator><creator>Pruski, Marek</creator><general>Royal Society of Chemistry</general><scope>NPM</scope><scope>AAYXX</scope><scope>CITATION</scope><scope>7X8</scope><scope>7SR</scope><scope>7U5</scope><scope>8BQ</scope><scope>8FD</scope><scope>JG9</scope><scope>L7M</scope><scope>OIOZB</scope><scope>OTOTI</scope></search><sort><creationdate>2016</creationdate><title>Effects of biradical deuteration on the performance of DNP: towards better performing polarizing agents</title><author>Perras, Frédéric A ; Reinig, Regina R ; Slowing, Igor I ; Sadow, Aaron D ; Pruski, Marek</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c486t-aa67f1691755be98fad8905e0da7edcbdf4e699bfd2a14246f9a75ed08c552203</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2016</creationdate><topic>Deuteration</topic><topic>Deuterium</topic><topic>Diffusion barriers</topic><topic>Dynamic tests</topic><topic>INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY</topic><topic>Polarization</topic><topic>Radicals</topic><topic>Saturation</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Perras, Frédéric A</creatorcontrib><creatorcontrib>Reinig, Regina R</creatorcontrib><creatorcontrib>Slowing, Igor I</creatorcontrib><creatorcontrib>Sadow, Aaron D</creatorcontrib><creatorcontrib>Pruski, Marek</creatorcontrib><creatorcontrib>Ames Lab., Ames, IA (United States)</creatorcontrib><collection>PubMed</collection><collection>CrossRef</collection><collection>MEDLINE - Academic</collection><collection>Engineered Materials Abstracts</collection><collection>Solid State and Superconductivity Abstracts</collection><collection>METADEX</collection><collection>Technology Research Database</collection><collection>Materials Research Database</collection><collection>Advanced Technologies Database with Aerospace</collection><collection>OSTI.GOV - Hybrid</collection><collection>OSTI.GOV</collection><jtitle>Physical chemistry chemical physics : PCCP</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Perras, Frédéric A</au><au>Reinig, Regina R</au><au>Slowing, Igor I</au><au>Sadow, Aaron D</au><au>Pruski, Marek</au><aucorp>Ames Lab., Ames, IA (United States)</aucorp><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Effects of biradical deuteration on the performance of DNP: towards better performing polarizing agents</atitle><jtitle>Physical chemistry chemical physics : PCCP</jtitle><addtitle>Phys Chem Chem Phys</addtitle><date>2016</date><risdate>2016</risdate><volume>18</volume><issue>1</issue><spage>65</spage><epage>69</epage><pages>65-69</pages><issn>1463-9076</issn><eissn>1463-9084</eissn><abstract>We study the effects of the deuteration of biradical polarizing agents on the efficiency of dynamic nuclear polarization (DNP) via the cross-effect. 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subjects | Deuteration Deuterium Diffusion barriers Dynamic tests INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY Polarization Radicals Saturation |
title | Effects of biradical deuteration on the performance of DNP: towards better performing polarizing agents |
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