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  • 1.
    Lindh, Erik L.
    et al.
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Applied Physical Chemistry. KTH, School of Chemical Science and Engineering (CHE), Centres, Wallenberg Wood Science Center.
    Bergenstråhle-Wohlert, Malin
    KTH, School of Chemical Science and Engineering (CHE), Centres, Wallenberg Wood Science Center.
    Terenzi, Camilla
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Applied Physical Chemistry. KTH, School of Chemical Science and Engineering (CHE), Centres, Wallenberg Wood Science Center.
    Salmén, Lennart
    KTH, School of Chemical Science and Engineering (CHE), Centres, Wallenberg Wood Science Center.
    Furó, Istvan
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Applied Physical Chemistry.
    Non-exchanging hydroxyl groups on the surface of cellulose fibrils: The role of interaction with water2016In: Carbohydrate Research, ISSN 0008-6215, E-ISSN 1873-426X, Vol. 434, p. 136-142Article in journal (Refereed)
    Abstract [en]

    The interaction of water with cellulose stages many unresolved questions. Here 2H MAS NMR and IR spectra recorded under carefully selected conditions in 1H-2H exchanged, and re-exchanged, cellulose samples are presented. It is shown here, by a quantitative and robust approach, that only two of the three available hydroxyl groups on the surface of cellulose fibrils are exchanging their hydrogen with the surrounding water molecules. This finding is additionally verified and explained by MD simulations which demonstrate that the 1HO(2) and 1HO(6) hydroxyl groups of the constituting glucose units act as hydrogen-bond donors to water, while the 1HO(3) groups behave exclusively as hydrogen-bond acceptors from water and donate hydrogen to their intra-chain neighbors O(5). We conclude that such a behavior makes the latter hydroxyl group unreactive to hydrogen exchange with water.

  • 2.
    Lindh, Erik L.
    et al.
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Applied Physical Chemistry.
    Salmén, Lennart
    KTH, School of Chemical Science and Engineering (CHE), Centres, Wallenberg Wood Science Center.
    Surface accessibility of cellulose fibrils studied by hydrogen-deuterium exchange with water2016In: Cellulose (London), ISSN 0969-0239, E-ISSN 1572-882X, Vol. 24, no 1, p. 21-33Article in journal (Refereed)
    Abstract [en]

    A problem with cellulose-based materials is that they are highly influenced by moisture, leading to reduced strength properties with increasing moisture content. By achieving a more detailed understanding of the water–cellulose interactions, the usage of cellulose-based materials could be better optimized. Two different exchange processes of cellulose hydroxyl/deuteroxyl groups have been monitored by transmission FT-IR spectroscopy. By using line-shape-assisted deconvolution of the changing intensities, we have been able to follow the exchange kinetics in a very detailed and controlled manner. The findings reveal a hydrogen exchange that mainly is located at two different kinds of fibril surfaces, where the differences arise from the water accessibility of that specific surface. The slowly accessible regions are proposed to be located between the fibrils inside of the aggregates, and the readily accessible regions are suggested to be at the surfaces of the fibril aggregates. It was also possible to identify the ratio of slowly and readily accessible surfaces, which indicated that the average aggregate of cotton cellulose is built up by approximately three fibrils with an assumed average size of 12 × 12 cellulose chains. Additionally, the experimental setup enabled visualizing and discussing the implications of some of the deviating spectral features that are pronounced when recording FT-IR spectra of deuterium-exchanging cellulose: the insufficient red shift of the stretching vibrations and the vastly decreasing line widths.

  • 3.
    Lindh, Erik L.
    et al.
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Applied Physical Chemistry.
    Terenzi, Camilla
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Applied Physical Chemistry.
    Furo, Istvan
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Applied Physical Chemistry.
    Salmén, Lennart
    KTH, School of Chemical Science and Engineering (CHE), Centres, Wallenberg Wood Science Center.
    Identifying different hydroxyl populations in cellulose by 2H MAS NMR2015In: Abstract of Papers of the American Chemical Society, ISSN 0065-7727, Vol. 249Article in journal (Other academic)
  • 4.
    Lindh, Erik L.
    et al.
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Applied Physical Chemistry. KTH, School of Chemical Science and Engineering (CHE), Centres, Wallenberg Wood Science Center.
    Terenzi, Camilla
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Applied Physical Chemistry. KTH, School of Chemical Science and Engineering (CHE), Centres, Wallenberg Wood Science Center.
    Salmén, Lennart
    KTH, School of Chemical Science and Engineering (CHE), Centres, Wallenberg Wood Science Center.
    Furo, Istvan
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Applied Physical Chemistry.
    Water in cellulose: evidence and identification of immobile and mobile adsorbed phases by H-2 MAS NMR2017In: Physical Chemistry, Chemical Physics - PCCP, ISSN 1463-9076, E-ISSN 1463-9084, Vol. 19, no 6, p. 4360-4369Article in journal (Refereed)
    Abstract [en]

    The organization of water molecules adsorbed onto cellulose and the supramolecular hydrated structure of microfibril aggregates represents, still today, one of the open and complex questions in the physical chemistry of natural polymers. Here, we investigate by H-2 MAS NMR the mobility of water molecules in carefully H-2-exchanged, and thereafter re-dried, microcrystalline cellulose. By subtracting the spectral contribution of deuteroxyls from the spectrum of hydrated cellulose, we demonstrate the existence of two distinct (H2O)-H-2 spectral populations associated with mobile and immobile water environments, between which the water molecules do not exchange at the NMR observation time scale. We conclude that those two water phases are located at differently-accessible adsorption sites, here assigned to the cellulose surfaces between and within the microfibril aggregates, respectively. The superior performance of H-2 MAS NMR encourages further applications of the same method to other complex systems that expose heterogeneous hygroscopic surfaces, like wood cell walls.

  • 5.
    Salmén, Lennart
    KTH, School of Chemical Science and Engineering (CHE), Centres, Wallenberg Wood Science Center. Innventia, Biorefinery & Biobased Mat, Stockholm, Sweden.
    Dynamic FTIR as a tool to assess the interaction of lignin in wood pulps2017In: Abstract of Papers of the American Chemical Society, ISSN 0065-7727, Vol. 253Article in journal (Other academic)
1 - 5 of 5
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