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Fabrication and mechanical characterization of graphene oxide-reinforced poly (acrylic acid)/gelatin composite hydrogelsThe mechanical performance of materials reinforced by cellulose nanofibrils is highly affected by the orientation of these fibrils. This paper investigates the nanofibril orientation distribution of films of partly oriented cellulose nanofibrils. Stripes of hydrogel films were subjected to different amount of strain and, after drying, examined with X-ray diffraction to obtain the orientation of the nanofibrils in the films, caused by the stretching. The cellulose nanofibrils had initially a random in-plane orientation in the hydrogel films and the strain was applied to the films before the nanofibrils bond tightly together, which occurs during drying. The stretching resulted in a reorientation of the nanofibrils in the films, with monotonically increasing orientation towards the load direction with increasing strain. Estimation of nanofibril reorientation by X-ray diffraction enables quantitative comparison of the stretch-induced orientation ability of different cellulose nanofibril systems. The reorientation of nanofibrils as a consequence of an applied strain is also predicted by a geometrical model of deformation of nanofibril hydrogels. Conversely, in high-strain cold-drawing of wet cellulose nanofibril materials, the enhanced orientation is promoted by slipping of the effectively stiff fibrils. V C 2015 AIP Publishing LLC. [http://dx.

The mechanical behaviour of cellulose nanofibrils is typically characterized by casting thin films and performing tensile tests on strips cut from these films. When comparing the stiffness of different films, the stiffness of the nanofibrils is only qualitatively and indirectly compared. This study provides some schemes based on various models of fibre networks, or laminated films, which can be used to assess the inherent stiffness of the nanofibrils from the stiffness of the films. Films of cellulose nanofibrils from different raw materials were manufactured and the elastic properties were measured. The expressions relating the nanofibril stiffness and the film stiffness were compared for the presented models. A model based on classical laminate theory showed the best balance between simplicity and adequacy of the underlying assumptions among the presented models. Using this model, the contributing nanofibril stiffness was found to range from 20 to 27 GPa. The nanofibril stiffness was also calculated from mechanical properties of nanofibril films found in the literature and compared with measurements from independent test methods of nanofibril stiffness. All stiffness values were found to be comparable and within the same order of magnitude.

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