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On cellulose dissolution and aggregation in aqueous tetrabutylammonium hydroxide

Author:
  • Marta Gubitosi
  • Hugo Duarte
  • Luigi Gentile
  • Ulf Olsson
  • Bruno Medronho
Publishing year: 2016-09-12
Language: English
Pages: 2873-2881
Publication/Series: Biomacromolecules
Volume: 17
Issue: 9
Document type: Journal article
Publisher: The American Chemical Society (ACS)

Abstract english

Aqueous tetrabutylammonium hydroxide, TBAH(aq), has been found to dissolve cellulose and to be a potential solvent for chemical processing or fiber spinning. In this paper, we have investigated the dissolution state of cellulose in 40 wt % TBAH(aq) solvent, and present an extensive study of rheology, combined with static light and small-angle X-ray scattering, to correlate cellulose aggregation with changes in the rheological parameters. Two cellulose molecular weights are compared. Microcrystalline cellulose (MCC), with a degree of polymerization of ca. 260, and a dissolving pulp with an approximately ten times higher molecular weight. Scattering data demonstrate that cellulose is molecularly dissolved at lower cellulose concentrations, while aggregates are present when the concentration exceeds a certain value. The onset of the aggregate formation is marked by a pronounced increase in the scattering intensity at low q, shear thinning behavior and violation of the empirical Cox-Merz rule. Additionally, the SAXS data suggest the presence of a solvation shell enriched in TBA+ ions, compared to the bulk solvent. The results are consistent with the recent suggestion that while native cellulose I may still dissolve, solutions are, above a particular concentration, becoming supersaturated with respect to the more stable crystal form cellulose II.

Keywords

  • Physical Chemistry

Other

Published
  • ISSN: 1525-7797
Luigi Gentile
E-mail: luigi [dot] gentile [at] fkem1 [dot] lu [dot] se

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MEMEG

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Physical Chemistry

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Research group

Microbial Ecology

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MICCS