Hampus Karlsson, Leo Svenningsson, Robin Storm, Poppy Chaiyupatham, Anders Brolin, Anette Larsson, Arthur C. Pinon, Staffan Schantz, Leif Karlson, Per A. Larsson, Lars Evenäs
{"title":"Dynamic nuclear polarization solid-state NMR spectroscopy as a tool to rapidly determine degree of modification in dialcohol cellulose","authors":"Hampus Karlsson, Leo Svenningsson, Robin Storm, Poppy Chaiyupatham, Anders Brolin, Anette Larsson, Arthur C. Pinon, Staffan Schantz, Leif Karlson, Per A. Larsson, Lars Evenäs","doi":"10.1007/s10570-024-06234-8","DOIUrl":null,"url":null,"abstract":"<div><p>Dialcohol cellulose can be prepared by periodate-mediated oxidation of cellulose followed by reduction with borohydride. The two-step reaction creates a modified cellulose polymer which is ring-opened between the C2 and C3 carbons in the glucose unit. This material has attracted both scientific and commercial interest, due to its potential role in the transition towards a fossil-fuel-free society. In order to become a reliable component in the materials of tomorrow, chemical properties such as degree of modification must be accurately quantified. In this work we describe how solid-state NMR spectroscopy, enhanced by dynamic nuclear polarization (DNP), can be used for this purpose. Our results illustrate that it is possible to obtain high sensitivity enhancements in dialcohol cellulose with the DNP enhanced solid-state NMR technique. Enhancements above a factor of fifty, on a 400 MHz/263 GHz DNP system in the presence of 12 mM AMUPol radical were achieved. This allows us to quantify the degree of modification in dialcohol cellulose samples in time spans as short as 20 min using DNP enhanced multiple-contact cross polarization experiments. We also exemplify how DNP enhanced, <sup>13</sup>C-<sup>13</sup>C dipolar recoupling experiments can be used for the same purpose and for studying chemical shift correlations in dialcohol cellulose.</p><h3>Graphical abstract</h3>\n<div><figure><div><div><picture><img></picture></div></div></figure></div></div>","PeriodicalId":511,"journal":{"name":"Cellulose","volume":"31 18","pages":"10727 - 10744"},"PeriodicalIF":4.9000,"publicationDate":"2024-10-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://link.springer.com/content/pdf/10.1007/s10570-024-06234-8.pdf","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Cellulose","FirstCategoryId":"88","ListUrlMain":"https://link.springer.com/article/10.1007/s10570-024-06234-8","RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"MATERIALS SCIENCE, PAPER & WOOD","Score":null,"Total":0}
引用次数: 0
Abstract
Dialcohol cellulose can be prepared by periodate-mediated oxidation of cellulose followed by reduction with borohydride. The two-step reaction creates a modified cellulose polymer which is ring-opened between the C2 and C3 carbons in the glucose unit. This material has attracted both scientific and commercial interest, due to its potential role in the transition towards a fossil-fuel-free society. In order to become a reliable component in the materials of tomorrow, chemical properties such as degree of modification must be accurately quantified. In this work we describe how solid-state NMR spectroscopy, enhanced by dynamic nuclear polarization (DNP), can be used for this purpose. Our results illustrate that it is possible to obtain high sensitivity enhancements in dialcohol cellulose with the DNP enhanced solid-state NMR technique. Enhancements above a factor of fifty, on a 400 MHz/263 GHz DNP system in the presence of 12 mM AMUPol radical were achieved. This allows us to quantify the degree of modification in dialcohol cellulose samples in time spans as short as 20 min using DNP enhanced multiple-contact cross polarization experiments. We also exemplify how DNP enhanced, 13C-13C dipolar recoupling experiments can be used for the same purpose and for studying chemical shift correlations in dialcohol cellulose.
期刊介绍:
Cellulose is an international journal devoted to the dissemination of research and scientific and technological progress in the field of cellulose and related naturally occurring polymers. The journal is concerned with the pure and applied science of cellulose and related materials, and also with the development of relevant new technologies. This includes the chemistry, biochemistry, physics and materials science of cellulose and its sources, including wood and other biomass resources, and their derivatives. Coverage extends to the conversion of these polymers and resources into manufactured goods, such as pulp, paper, textiles, and manufactured as well natural fibers, and to the chemistry of materials used in their processing. Cellulose publishes review articles, research papers, and technical notes.