From a circular economy perspective, one-pot strategies for the isolation of cellulose nanomaterials at a high yield and with multifunctional properties are attractive. Here, the effects of lignin content (bleached vs unbleached softwood kraft pulp) and sulfuric acid concentration on the properties of crystalline lignocellulose isolates and their films are explored. Hydrolysis at 58 wt % sulfuric acid resulted in both cellulose nanocrystals (CNCs) and microcrystalline cellulose at a relatively high yield (>55%), whereas hydrolysis at 64 wt % gave CNCs at a lower yield (<20%). CNCs from 58 wt % hydrolysis were more polydisperse and had a higher average aspect ratio (1.5-2×), a lower surface charge (2×), and a higher shear viscosity (100-1000×). Hydrolysis of unbleached pulp additionally yielded spherical nanoparticles (NPs) that were <50 nm in diameter and identified as lignin by nanoscale Fourier transform infrared spectroscopy and IR imaging. Chiral nematic self-organization was observed in films from CNCs isolated at 64 wt % but not from the more heterogeneous CNC qualities produced at 58 wt %. All films degraded to some extent under simulated sunlight trials, but these effects were less pronounced in lignin-NP-containing films, suggesting a protective feature, but the hemicellulose content and CNC crystallinity may be implicated as well. Finally, heterogeneous CNC compositions obtained at a high yield and with improved resource efficiency are suggested for specific nanocellulose uses, for instance, as thickeners or reinforcing fillers, representing a step toward the development of application-tailored CNC grades. © 2023 The Authors. 

The biotechnological applications of cellulose nanocrystals (CNCs) continue to grow due to their sustainable nature, impressive mechanical, rheological, and emulsifying properties, upscaled production capacity, and compatibility with other materials, such as protein and polysaccharides. In this study, hydrogels from CNCs and pectin, a plant cell wall polysaccharide broadly used in food and pharma, were produced by calcium ion-mediated internal ionotropic gelation (IG). In the absence of pectin, a minimum of 4 wt% CNC was needed to produce self-supporting gels by internal IG, whereas the addition of pectin at 0.5 wt% enabled hydrogel formation at CNC contents as low as 0.5 wt%. Experimental data indicate that CNCs and pectin interact to give robust and self-supporting hydrogels at solid contents below 2.5 %. Potential applications of these gels could be as carriers for controlled release, scaffolds for cell growth, or wherever else distinct and porous network morphologies are required.

Conversion of biomass to biofuels and other products is a research area that is currently attracting a great amount of interest, particularly because such production may be envisaged as a key part of any bio-based economy. Lignocellulosic biomass is abundant and sustainable, and can therefore potentially support large-scale production of biofuel as an alternative to petroleum-based fuel.

The enzymatic hydrolysability of three industrial pulps, five lab made pulps, and one microcrystalline cellulose powder was assessed using commercial cellulolytic enzymes. To gain insight into the factors that influence the hydrolysability, a thorough characterization of the samples was done, including their chemical properties (cellulose content, hemicellulose content, lignin content, and kappa number), their macromolecular properties (peak molar mass, number-average molar mass, weight-average molar mass, polydispersity, and limiting viscosity) and their supramolecular properties (fibre saturation point, specific surface area, average pore size, and crystallinity). The hydrolysability was assessed by determination of initial conversion rate and final conversion yield, with conversion yield defined as the amount of glucose in solution per unit of glucose in the substrate. Multivariate data analysis revealed that for the investigated samples the conversion of cellulose to glucose was mainly dependent on the supramolecular properties, such as specific surface area and average pore size. The molar mass distribution, the crystallinity, and the lignin content of the pulps had no significant effect on the hydrolysability of the investigated samples.

In addition, experiments were carried out aiming at identifying suitable conditions for pre-treatment of wheat straw, for the purpose of making cellulose rich pulps with improved enzymatic reactivity. Two sets of conditions for pre-treatment of wheat straw were identified; a combination of low temperature alkaline washing and acid pre-hydrolysis, or high temperature acid pre-hydrolysis. Both bleached wheat straw pulps showed similar enzymatic reactivity. However, the enzymatic reactivity of both bleached wheat straw pulps was found to be significantly less than what has been achieved for wood pulps. A probable explanation for the low enzymatic reactivity of the bleached wheat straw pulp can be the small pore size, limiting the access for enzymes to the cellulose surfaces in the fibre wall interior.Text, figures and tables in an extended abstract (< 4 pages with title and references).

The enzymatic hydrolysability of three industrial pulps, five lab made pulps, and one microcrystalline cellulose powder was assessed using commercial cellulolytic enzymes. To gain insight into the factors that influence the hydrolysability, a thorough characterization of the samples was done, including their chemical properties (cellulose content, hemicellulose content, lignin content, and kappa number), their macromolecular properties (peak molar mass, number-average molar mass, weight-average molar mass, polydispersity, and limiting viscosity) and their supramolecular properties (fibre saturation point, specific surface area, average pore size, and crystallinity). The hydrolysability was assessed by determination of initial conversion rate and final conversion yield, with conversion yield defined as the amount of glucose in solution per unit of glucose in the substrate. Multivariate data analysis revealed that for the investigated samples the conversion of cellulose to glucose was mainly dependent on the supramolecular properties, such as specific surface area and average pore size. The molar mass distribution, the crystallinity, and the lignin content of the pulps had no significant effect on the hydrolysability of the investigated samples.

A study has been made of several aspects of determination of ash content in kraft lignin samples using thermogravimetric analysis (TGA). Three different methods were used; with the main differences between the methods being that two have a temperature hold at 250 deg C to remove volatiles and that the three methods use different maximum temperatures, namely 525, 550 and 575 deg C, respectively. The three kraft lignins used were produced using the LignoBoost lignin isolation process. It has been demonstrated that the results obtained by the different temperature programmes showed no significant difference. The results were comparable with those from using oven ignition. Moreover, the limit of quantification was several orders of magnitude lower than when using oven ignition. It has been recommended that if TGA is used for determination of ash content, a temperature programme from a standard method should be used, which should be mentioned together with the results. The temperature programme in method one (corresponding to ISO 1762) was the shortest and the preferable method. A well as requiring less labour due to fewer movements in the analytical protocol, the TGA methods enabled a high sample throughput due to autosampling possibilities.

Thermogravimetric analysis (TGA) in oxidative conditions is a promising alternative to ignition in oven for the determination of inorganic residue, commonly referred to as ash. It is here shown that TGA can be used with temperature programs resembling those in standardized methods for oven ignition, and obtainequivalent results even though the sample amount is several orders of magnitude lower. The precision and limit of quantification of TGA is also discussed.

The effect of initial stages of pulping of spruce, resembling prehydrolysis and alkaline cooking was studied using CP/MAS 13C-NMR, X-ray scattering, FSP and carbohydrate composition in order to study the impact of the pre-treatments on the fiber wall nanostructure. Removal of fiber wall components, hemicellulose and lignin, increased the fiber wall porosity and induced cellulose fibril aggregation. The effect of temperature and pH in the treatment on cellulose fibril aggregate size appears to be secondary. It is the removal of hemicellulose that has a profound effect on the supramolecular structure of the cellulose fiber wall. As the amount of hemicellulose dissolved from wood increases, the fibril aggregate size determined by NMR increases as well, ranging from 16 to 28 nm. Specifically, a good correlation between the amount of glucomannan in the fiber wall and the fibril aggregate size is seen. The lower the amount of glucomannan, the larger the aggregate size. Glucomannan thus seems to prevent aggregation as it acts as a very efficient spacer between fibrils. Elemental fibril size determined by NMR, was quite similar for all samples, ranging from 3.6 to 4.1 nm. By combining measurement methods, a more well-resolved picture of the structural changes occurring during was obtained. © 2021, The Author(s).

To commercialize a biomedical product as a medical device, reproducibility of production and time-stability are important parameters. Studies of reproducibility are lacking in the literature. Additionally, chemical pre-treatments of wood fibres to produce highly fibrillated cellulose nanofibrils (CNF) seem to be demanding in terms of production efficiency, being a bottleneck for industrial upscaling. In this study, we evaluated the effect of pH on the dewatering time and washing steps of 2,2,6,6-Tetramethylpiperidinyloxy (TEMPO)-mediated oxidized wood fibres when applying 3.8 mmol NaClO/g cellulose. The results indicate that the method does not affect the carboxylation of the nanocelluloses, and levels of approximately 1390 μmol/g were obtained with good reproducibility. The washing time of a Low-pH sample was reduced to 1/5 of the time required for washing a Control sample. Additionally, the stability of the CNF samples was assessed over 10 months and changes were quantified, the most pronounced were the increase of potential residual fibre aggregates, reduction of viscosity and increase of carboxylic acid content. The cytotoxicity and skin irritation potential were not affected by the detected differences between the Control and Low-pH samples. Importantly, the antibacterial effect of the carboxylated CNFs against S. aureus and P. aeruginosa was confirmed. © 2023 The Authors

Cellulose nanofibrils (CNFs) were obtained by applying a chemical pretreatment consisting of autoclaving the pulp fibers in sodium hydroxide, combined with 2,2,6,6-tetramethylpiperidinyl-1-oxyl-mediated oxidation. Three levels of sodium hypochlorite were applied (2.5, 3.8, and 6.0 mmol/g) to obtain CNF qualities (CNF_2.5, CNF_3.8, and CNF_6.0) with varying content of carboxyl groups, that is, 1036, 1285, and 1593 μmol/g cellulose. The cytotoxicity and skin irritation potential (indirect tests) of the CNFs were determined according to standardized in vitro testing for medical devices. We here demonstrate that autoclaving (121 °C, 20 min), which was used to sterilize the gels, caused a modification of the CNF characteristics. This was confirmed by a reduction in the viscosity of the gels, a morphological change of the nanofibrils, by an increase of the ultraviolet-visible absorbance maxima at 250 nm, reduction of the absolute zeta potential, and by an increase in aldehyde content and reducing sugars after autoclaving. Fourier-transform infrared spectroscopy and wide-angle X-ray scattering complemented an extensive characterization of the CNF gels, before and after autoclaving. The antibacterial properties of autoclaved carboxylated CNFs were demonstrated in vitro (bacterial survival and swimming assays) on Pseudomonas aeruginosa and Staphylococcus aureus. Importantly, a mouse in vivo surgical-site infection model on S. aureus revealed that CNF_3.8 showed pronounced antibacterial effect and performed as good as the antiseptic Prontosan wound gel.

Correction for ‘One-shot carboxylation of microcrystalline cellulose in the presence of nitroxyl radicals and sodium periodate’ by Sergiu Coseri et al., RSC Adv., 2015, 5, 85889–85897.

The authors regret that the images presented for Fig. 1 and 3 in the original article present incorrect carbohydrate structures. The amended versions of these images, in which the 3-position hydroxyl groups are equatorial rather than axial, are presented below.

Water soluble cellulose derivatives are highly required products for many practical purposes, expanding the limited applications of pure cellulose caused by the highly ordered hydrogen bond network and high crystallinity. In this connection, this paper, presents a new approach to obtain water soluble carboxyl-functionalized cellulosic materials, combining two of the most common selective oxidation protocols for cellulose, i.e. nitroxyl mediated reaction and periodate oxidation, in a one-shot reaction. It was found that, under specific reaction conditions, fully oxidized, 2,3,6-tricarboxy cellulose can be obtained in large amounts. The other valuable oxidized fractions were found to possess large amounts of carboxylic groups, as determined by potentiometric titration. 13C-NMR evidenced the presence of three distinctive carboxylic groups in the fully oxidized product, whereas for the partially oxidized samples, 13C CP-MAS solid-state NMR did not detect any carbonyl signals. The oxidized products were characterized by means of FTIR and X-ray photoelectron spectroscopy (XPS). Moreover, the changes of the degree of polymerization occurring after oxidative treatments were viscometrically determined.

The effect on softwood fiber wall nanostructure of kraft cooking, oxygen delignification and refining was evaluated by X-ray scattering. A recently developed simulation method for modelling small angle X-ray scattering (SAXS) data was used to estimate the apparent average sizes of solids (AAPS) and interstitial spaces in the fiber wall (AACS). Fiber saturation point and wide angle X-ray scattering were also used to calculate the pore volume in the fiber wall and the crystallite size of the fibril, respectively. The experimental modelled SAXS data was able to give consistent values for each kraft-cooked and oxygen-delignified pulp. Kraft delignification seems to have the major influence on the fiber nanostructure modification, while oxygen delignification has little or no significant impact even for different kappa numbers. The particle sizes values were more stable than the cavities sizes and no significant differences were seen between different delignification processes, refining or delignification degree. Pulps evaluated after PFI-refining, showed an increase in the fiber wall porosity evaluated by FSP and an increase in the interstitial spaces in the fiber wall, while the crystallite size and the particle sizes were very little or not affected at all. 

An important traditional load bearing member in oriental ancient timber structure buildings, i.e. Huagong (flower arm), was selected to explore the alterations in cell wall components and hygroscopic properties of wood during long time ageing. This archaeological poplar (Populus spp.) wood with cal. BP 690: BP 790 was studied from the wood surface and inwards by means of imaging FTIR spectroscopy, X-ray diffraction and dynamic vapour sorption. The deterioration of the archaeological wood mainly displayed a depolymerization of glucomannan and lignin as well as a hydrolysis of the glucuronic acid of xylan and of the aromatic C–O groups in the condensed lignins or lignin–carbohydrate complexes. Furthermore, the degradation promoted the rearrangement of the cellulose molecules in adjacent microfibrils. The cellulose crystallites in the archaeological wood were therefore packed more tightly and had larger diameter. The structural alterations of wood cell wall components and a decrease in crystallinity contributed to an increase in the number of moisture bonding sites and led to an increase in both the equilibrium moisture content of the archaeological wood in the entire RH range as well as an increase in hysteresis.

A simulation method was developed for modelling SAXS data recorded on cellulose rich pulps. The modelling method is independent of the establishment of separate form factors and structure factors and was used to model SAXS data recorded on dense samples. An advantage of the modelling method is that it made it possible to connect experimental SAXS data to apparent average sizes of particles and cavities at different sample solid contents. Experimental SAXS data could be modelled as a superposition of a limited number of simulated intensity components and gave results in qualitative agreement with CP/MAS 13C-NMR data recorded on the same samples. For the water swollen samples, results obtained by the SAXS modelling method and results obtained from CP/MAS 13C-NMR measurements, agreed on the ranking of particle sizes in the different samples. The SAXS modelling method is dependent on simulations of autocorrelation functions and the time needed for simulations could be reduced by rescaling of simulated correlation functions due to their independence of the choice of step size in real space. In this way an autocorrelation function simulated for a specific sample could be used to generate SAXS intensity profiles corresponding to all length scales for that sample and used for efficient modelling of the experimental data recorded on that sample. Graphical abstract: [Figure not available: see fulltext.] © 2021, The Author(s).

Cellulose rich and cellulose enriched pulps are com. important and scientifically interesting materials with a complex hierarchical fiber wall nanostructure which change with moisture sorption and swelling in water. The fiber wall building blocks and cavities are in size ranges addressable by small angle x-ray scattering (SAXS) but due to large variability in sizes and shapes, extracting quant. data about the fiber wall nanostructure from SAXS data can be challenging. For this purpose, a simulation method was developed for modeling SAXS data recorded on cellulose rich pulps. The modeling method is independent of the establishments of sep. form factors and structure factors and was used to model SAXS data recorded on dense samples. An advantage of the modeling method was that it made it possible to connect exptl. SAXS data to apparent average sizes of particles and cavities at different sample solid contents. Exptl. SAXS data could be modelled as a superposition of a limited number of simulated intensity components and gave results in qual. agreement with CP/MAS 13C-NMR data recorded on the same samples. For the water swollen samples, results obtained by the SAXS modeling method and results obtained from CP/MAS 13C-NMR measurements, agreed on the ranking of particle sizes in the different samples. The SAXS modeling method is dependent on simulations of autocorrelation functions. The time needed for simulations could be reduced by rescaling of simulated correlation functions, due to their independence of the choice of step size in real space. This way an autocorrelation function simulated for a specific sample could be used to generate SAXS intensity profiles corresponding to all length scales for that sample and used for efficient modeling of the exptl. data recorded on that sample.

The impact of the size of the charged group on the properties of alkoxylated NFC was studied by two chloroalkyl acid reagents. It was found that the employment of the larger 2-chloropropionic acid reagent leads to improved properties, e.g. higher fraction of nano-sized materials, and significantly better redispersion as compared to when the smaller monochloroacetic acid was employed. The differences in the impacts of the different reagents were hypothesized to be due to a more efficient disruption of the cohesion between the nanofibrils when a larger charged group was employed. 

 For the first time in the Bioeconomy research program at RISE, corrugatedboard has an own research area. Research is building around the main driving forcesin the corrugated board value chain like e-commerce, improved box performance anddigital printing. The main weakness of corrugated board, its moisture sensitivity, isalso addressed.These main driving forces and weaknesses of corrugated board are mirrored in thethemes of this large research program area:Fibre sorption and deformation mechanismsFundamental knowledge on the mechanisms behind moisture sorption and deformation on fibre level is developed to increase moisture and creep resistance throughmodification of paper materials. State of the art methods for characterization ofthe fibre ultra- and nano-structure such as Fourier transform infra-red spectroscopy(FTIR), small angle X-ray scattering (SAXS), and wide angle X-ray scattering (WAXS)give new insights on mechanisms and clarify effects of moisture as well as chemicalmodifications.Papermaking for improved base sheetsConcepts that are explored are fibre-based strength additives produced with novelrefining techniques, and modified ZD-profiles in the sheet for better mechanical properties.Box mechanicsMechanical performance of structures such as corrugated board boxes can be predicted through physically based mathematical modelling by taking the behaviour ofthe constituent materials as well as the geometry into account. Appropriate materialmodels for the corrugated board are identified and finite element models for simulation of corrugated board packaging performance are developed.Tool for inkjet printability on corrugatedThere is a genuine need for improved inkjet printability on corrugated materials thanksto rapid development in e-commerce as well as digitalization along the corrugatedvalue chain. Effective measurement methods and knowledge around ink-substrateinteractions are developed to enable board producers and converters to have effective product development and predictable printability on not only liners but also oncorrugated materials.

Main conclusion: Glucomannan was more strongly oriented, in line with the orientation of cellulose, than the xylan in both compression wood and normal wood of Chinese fir. Lignin in compression wood was somewhat more oriented in the direction of the cellulose microfibrils than in normal wood. The structural organization in compression wood (CW) is quite different from that in normal wood (NW). To shed more light on the structural organization of the polymers in plant cell walls, Fourier Transform Infrared (FTIR) microscopy in transmission mode has been used to compare the S2-dominated mean orientation of wood polymers in CW with that in NW from Chinese fir (Cunninghamia lanceolata). Polarized FTIR measurements revealed that in both CW and NW samples, glucomannan and xylan showed a parallel orientation with respect to the cellulose microfibrils. In both wood samples, the glucomannan showed a much greater degree of orientation than the xylan, indicating that the glucomannan has established a stronger interaction with cellulose than xylan. For the lignin, the absorption peak also indicated an orientation along the direction of the cellulose microfibrils, but this orientation was more pronounced in CW than in NW, indicating that the lignin is affected by the orientation of the cellulose microfibrils more strongly in CW than it is in NW.

Glucomannan was more strongly oriented, in line with the orientation of cellulose, than the xylan in both compression wood and normal wood of Chinese fir. Lignin in compression wood was somewhat more oriented in the direction of the cellulose microfibrils than in normal wood.

The structural organization in compression wood (CW) is quite different from that in normal wood (NW). To shed more light on the structural organization of the polymers in plant cell walls, Fourier Transform Infrared (FTIR) microscopy in transmission mode has been used to compare the S₂-dominated mean orientation of wood polymers in CW with that in NW from Chinese fir (Cunninghamia lanceolata). Polarized FTIR measurements revealed that in both CW and NW samples, glucomannan and xylan showed a parallel orientation with respect to the cellulose microfibrils. In both wood samples, the glucomannan showed a much greater degree of orientation than the xylan, indicating that the glucomannan has established a stronger interaction with cellulose than xylan. For the lignin, the absorption peak also indicated an orientation along the direction of the cellulose microfibrils, but this orientation was more pronounced in CW than in NW, indicating that the lignin is affected by the orientation of the cellulose microfibrils more strongly in CW than it is in NW.

Heat treatment is a promising pre-processing method in the conversion of kraft lignins to carbon fibers. In this study, a kraft lignin was subjected to heat treatment at different lengths of time and at different temperatures. The molecular structure of the untreated and four heat treated lignins were investigated mainly by a variety of nuclear magnetic resonance spectroscopy (NMR) methods. The results were compared to structural information obtained by pyrolysis-gas chromatography-/mass spectrometry (py-GC/MS) and Fourier transform infrared spectroscopy (FTIR). It was observed that during the thermal treatment, the amount of β-O-4 ether moieties decreased, and an intramolecular conversion of secoisolariciresinol residues to cyclic ethers occurred. The effects on shape and size of the lignins were investigated by size exclusion chromatography (SEC) and NMR-diffusion measurements, by which the hydrodynamic radii were found to increase as a result of thermal treatment. It is discussed whether this depends on reduced flexibility and/or increased molar mass. In addition, the trends from the SEC and NMR analyses were compared to changes in glass transition temperature as determined by differential scanning calorimetry (DSC).

Drying of chemical pulps results in a decreased swelling of the fibres, leading to lower density and strength properties of paper sheets. To investigate how variation of pulp pH, drying process temperature, and final moisture content affect this phenomenon, structural studies were performed on a cellulose-rich pulp. Interrupting the drying at moisture contents of around 20%, using drying temperatures of 80 °C and 140 °C, resulted in a more severe degree of hornification than if the pulp was completely dried at the same temperatures. This increased loss of swelling was accompanied by increased cellulose microfibril aggregation. No change of the cellulose microfibril size or of the cellulose crystallinity, as determined by NMR, could be seen. Further, the accessibility of the cellulose microfibril surfaces, including surfaces between microfibrils, was unaffected by the drying. Thus, hornification should not primarily be related to a reduction of accessible cellulosic surfaces.

Abstract: Moisture absorption in the cell wall structure of wood is well known to induce considerable swelling of the wood exerting high expansion forces. This swelling is mainly induced by the sorptive action of the hydroxyl groups of the carbohydrate wood polymers; cellulose and hemicelluloses. On the ultrastructural level, there are, however, still questions with regard to the detailed deformations induced by this moisture absorption. Here, FTIR spectroscopy and synchrotron-radiation-based X-ray diffraction were used on paper samples to study the deformation of the cellulose crystals as a consequence of moisture absorption and desorption. Both techniques revealed that the moisture absorption resulted in a transverse contraction of the cellulose crystals accompanied by a somewhat smaller elongation in the cellulose chain direction. The deformations were found to be a direct response to the increased moisture content and were also found to be reversible during moisture desorption. It is hypothesised that these deformations are a consequence of the swelling forces created by the combined longitudinal and lateral expansions of the non-crystalline cellulose molecules and the glucomannan hemicellulose aligned along the cellulose crystals. These forces will impose a lateral contraction of the cellulose crystals, as well as a longitudinal extension of it. Graphic abstract: [Figure not available: see fulltext.]. © 2021, The Author(s).

A deeper insight into the molecular interactions in the highly intermixed structure of the wood cell wall, from the point of view of both basic and applied science, is necessary. In particular, the role of the different matrix materials within the cell wall needs to be better understood, especially concerning how lignin contributes to the mechanical properties. In the present paper, the mechanical properties of spruce wood have been studied on a molecular scale by means of dynamic Fourier transform infrared (FTIR) spectroscopy. To this purpose, native spruce wood was subjected to chemical changes by impregnation and a mild pre-cooking with white liquor with a composition usual for kraft pulping. For comparison, lignin-rich primary cell wall material was also isolated by means of thermomechanical pulp (TMP) refining. Dynamic FTIR spectroscopy revealed that lignin took part in the stress transfer in all investigated samples. This finding is in contrast to literature data. A strong indirect coupling between lignin and cellulose was seen in the primary cell wall (P) material. In case of native wood, the lignin signal was much weaker and also indicated an indirect coupling to cellulose. In the case of pre-cooked wood samples (submitted to mild pulping), the interactions were modified so that the molecular straining of lignin was stronger and more directly related to that of cellulose. In other words, in these samples, lignin played a more active role in the stress transfer as compared to native wood. These findings were supported by a narrower lignin-softening region as measured by dynamic mechanical analysis (DMA). The interpretation is plausible in terms of the superior stiffness seen for high-yield pulps of a similar yield as the studied pre-cooked wood samples.

Mechano-sorptive creep, i.e. the increased rate of creep that occurs during changing relative humidity, when loading paper or wood, is a phenomenon still not fully understood. This phenomenon was here investigated by examining the changes occurring at the molecular level utilising FTIR spectroscopy. By subjecting the paper to deuterated water, the changes involving both the crystalline hydroxyls as well as those in accessible regions could be examined. During loading, the cellulose molecular chains are stretched taking the load. In addition, during mechano-sorptive creep a further exchange from OH to OD groups occurred. This was interpreted as caused by slippage between cellulose fibrils allowing previously non-accessible hydroxyls to become available for deuterium exchange. Thus, the loosening of the structure, during the changing moisture conditions, is interpreted as what has led to the increased creep and the possibility for new areas of cellulose fibril/fibril aggregates to be exposed to the deuterium exchange.