This paper reports a nontoxic, soft and electroactive hydrogel made with polyvinyl alcohol (PVA) and cellulose nanocrystal (CNC). The CNC incorporating PVA-CNC hydrogels were prepared using a freeze–thaw technique with different CNC concentrations. Fourier transform infrared spectroscopy, thermogravimetric analysis, X-ray diffraction and scanning electron microscopy results proved the good miscibility of CNCs with PVA. The optical transparency, water uptake capacity and mechanical properties of the prepared hydrogels were investigated in this study. The CNC incorporating PVA-CNC hydrogels showed improved displacement output in the presence of an electric field and the displacement increased with an increase in the CNC concentration. The possible actuation mechanism was an electrostatic effect and the displacement improvement of the hydrogel associated with its enhanced dielectric properties and softness. Since the prepared PVA-CNC hydrogel is nontoxic and electroactive, it can be used for biomimetic soft robots, actively reconfigurable lenses and active drug-release applications.

Cellulose nanofiber (CNF) exhibits excellent mechanical properties, which has been extensively proven through experimental techniques. However, understanding the mechanisms and the inherent structural behavior of cellulose is important in its vastly growing research areas of applications. This study focuses on taking a look into what happens to the atomic molecular interactions of CNF, mainly hydrogen bond, in the presence of external force. This paper investigates the hydrogen bond disparity within CNF structure. To achieve this, molecular dynamics simulations of cellulose I $\beta$ nanofibers are carried out in equilibrated conditions in water using GROMACS software in conjunction with OPLS-AA force field. It is noted that the hydrogen bonds within the CNF are disrupted when a pulling force is applied. The simulated Young’s modulus of CNF is found to be 161 GPa. A simulated shear within the cellulose chains presents a trend with more hydrogen bond disruptions at higher forces.

The alignment of cellulose by an electric field is an interesting subject for cellulose material processing and its applications. This paper reports an atomistic molecular dynamics simulation of the crystalline cellulose nanofiber (CNF) model in varying electric field directions and strengths. GROMACS software was used to study crystalline cellulose 1β consisting of 18 chains in an aqueous environment at room temperature, and an electric field was applied along the cellulose chain direction and the perpendicular direction with varying field strength. The root-mean-square displacement, radius of gyration, end-to-end length, and hydrogen bond population of the crystalline CNF model were analyzed to determine the effects of the applied electric field on the structure of the CNF model. The results suggest that the nanosecond electric field can induce the orientation of the CNF along the applied electric field direction. The alignment rate and ability to maintain the alignment depend on the electric field strength. Analysis of the radius of gyration, end-to-end length, and bond lengths for intrachain and interchain hydrogen bonds revealed no significant effect on the cellulose structure. Cellulose alignment in an electric field has the potential to broaden the design of electric field-induced processing techniques for cellulose filaments, thin films, and electro-active cellulose composites.

This paper reports a genuine environment-friendly hybrid nanocomposite made by growing zinc oxide (ZnO) nanorods on cellulose nanofiber (CNF) film. The nanocomposite preparation, characterizations, electromechanical property, and ultraviolet (UV) sensing performance are explained. CNF was extracted from the pulp by combining the 2,2,6,6-tetramethylpiperidine-1-oxyl radical (TEMPO) oxidation and the aqueous counter collision (ACC) methods. The CNF film was fabricated using doctor blade casting, and ZnO nanorods were grown on the CNF film by seeding and by a hydrothermal method. Morphologies, optical transparency, mechanical and electromechanical properties, and UV sensing properties were examined. The nanocomposite’s optical transparency was more than 80%, and the piezoelectric charge constant d₃₁ was 200 times larger than the CNF film. The UV sensing performance of the prepared ZnO-CNF nanocomposites was tested in terms of ZnO concentration, UV irradiance intensity, exposure side, and electrode materials. A large aspect ratio of ZnO nanorods and a work function gap between ZnO nanorods and the electrode material are essential for improving the UV sensing performance. However, these conditions should be compromised with transparency. The use of CNF for ZnO-cellulose hybrid nanocomposite is beneficial not only for electromechanical and UV sensing properties but also for high mechanical properties, renewability, biocompatibility, flexibility, non-toxicity, and transparency.

Polycaprolactone (PCL) is a semicrystalline thermoplastic polymer well-known as a nontoxic and biodegradable material. Due to this nature, PCL has been studied for drug delivery and a bioscaffold in tissue engineering. However, it has incomplete properties as the structural materials such as relatively low mechanical properties, low surface energy, and long degradation rates. Thus, this study aims to complement the previous shortcomings and present the possibility of a more advanced biomaterial by forming nanocomposites with cellulose nanocrystal (CNC), one of the abundant natural polymers with high specific modulus and strength, environmentally-friendliness, and nontoxic. Bulk materials with various concentrations of CNC in PCL matrix were fabricated, and a three-point bending test was conducted. The measured bending modulus was compared with the estimated values based on the rule of mixtures of the nanocomposite and surface morphology was investigated by scanning electron microscopy.