Dynamic nuclear polarization solid-state NMR spectroscopy as a tool to rapidly determine degree of modification in dialcohol cellulose
Journal article, 2024
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. Graphical abstract: (Figure presented.).
Renewable thermoplastics
Solid-state NMR
Degree of modification
Dynamic nuclear polarization
Dialcohol cellulose
Author
Hampus Karlsson
Chalmers, Chemistry and Chemical Engineering, Applied Chemistry
Leo Svenningsson
Chalmers, Chemistry and Chemical Engineering, Applied Chemistry
Robin Storm
Chalmers, Chemistry and Chemical Engineering, Applied Chemistry
Poppy Thanaporn Chaiyupatham
Chalmers, Chemistry and Chemical Engineering, Applied Chemistry
Anders Brolin
Royal Institute of Technology (KTH)
Stora Enso AB
Anette Larsson
Chalmers, Chemistry and Chemical Engineering, Applied Chemistry
Arthur C. Pinon
University of Gothenburg
Staffan Schantz
AstraZeneca AB
University of Gothenburg
Leif Karlson
Nouryon
Per A. Larsson
Royal Institute of Technology (KTH)
Lars Evenäs
Chalmers, Chemistry and Chemical Engineering, Applied Chemistry
Cellulose
0969-0239 (ISSN) 1572882x (eISSN)
Vol. 31 18 10727-10744Subject Categories (SSIF 2011)
Polymer Chemistry
Paper, Pulp and Fiber Technology
Other Chemistry Topics
DOI
10.1007/s10570-024-06234-8
Related datasets
Dynamic nuclear polarization solid-state NMR spectroscopy as a tool to rapidly determine degree of modification in dialcohol cellulose [dataset]
DOI: 10.5281/zenodo.13341684