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Atomic resolution of cotton cellulose structure enabled by dynamic nuclear polarization solid-state NMR

Authors
  • Kirui, Alex1
  • Ling, Zhe2, 3
  • Kang, Xue1
  • Dickwella Widanage, Malitha C.1
  • Mentink-Vigier, Frederic4
  • French, Alfred D.2
  • Wang, Tuo1
  • 1 Louisiana State University, Department of Chemistry, Baton Rouge, LA, 70803, USA , Baton Rouge (United States)
  • 2 Southern Regional Research Center USDA, New Orleans, LA, 70124, USA , New Orleans (United States)
  • 3 Beijing Forestry University, Beijing, 100083, People’s Republic of China , Beijing (China)
  • 4 National High Magnetic Field Laboratory, Tallahassee, FL, 32310, USA , Tallahassee (United States)
Type
Published Article
Journal
Cellulose
Publisher
Springer-Verlag
Publication Date
Nov 11, 2018
Volume
26
Issue
1
Pages
329–339
Identifiers
DOI: 10.1007/s10570-018-2095-6
Source
Springer Nature
Keywords
License
Yellow

Abstract

AbstractThe insufficient resolution of conventional methods has long limited the structural elucidation of cellulose and its derivatives, especially for those with relatively low crystallinities or in native cell walls. Recent 2D/3D solid-state NMR studies of 13C uniformly labeled plant biomaterials have initiated a re-investigation of our existing knowledge in cellulose structure and its interactions with matrix polymers but for unlabeled materials, this spectroscopic method becomes impractical due to limitations in sensitivity. Here, we investigate the molecular structure of unlabeled cotton cellulose by combining natural abundance 13C–13C 2D correlation solid-state NMR spectroscopy, as enabled by the sensitivity-enhancing technique of dynamic nuclear polarization, with statistical analysis of the observed and literature-reported chemical shifts. The atomic resolution allows us to monitor the loss of Iα and Iβ allomorphs and the generation of a novel structure during ball-milling, which reveals the importance of large crystallite size for maintaining the Iα and Iβ model structures. Partial order has been identified in the “disordered” domains, as evidenced by a discrete distribution of well-resolved peaks. This study not only provides heretofore unavailable high-resolution insights into cotton cellulose but also presents a widely applicable strategy for analyzing the structure of cellulose-rich materials without isotope-labeling. This work was part of a multi-technique study of ball-milled cotton described in the previous article in the same issue.Graphical abstract

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