Cellulose, the chain of glucose residues easily obtained from nature, is the most common natural polymer. Owing to its own unique material properties, compared to the conventional usage, nanocellulose (NC) with a crystalline structure can be considered to be used in various industrial applications. As a novel sustainable future material, we review the recent achievements of NC from the view point of material extraction and the composite processes to some extended important applications. While the mechanical properties of NCs and the energy consumption during their composite processing are the key considerations, their application potentials have never been limited to mechanical or commodity products as conventional celluloses. In the latter part of this review, emerging engineering applications of NCs such as energy storage, flexible electronics, and smart materials will be further discussed for readers searching future high-end eco-friendly functional materials. Also some suggestions for potential applications will be also discussed.

Natural melanins are biocompatible conductors with versatile functionalities. Here, we report fabrication of multifunctional poly(vinyl alcohol)/melanin nanocomposites by layer-by-layer (LBL) assembly using melanin nanoparticles (MNPs) directly extracted from sepia officinalis inks. The LBL assembly offers facile manipulation of nanotextures as well as nm-thickness control of the macroscale film by varying solvent qualities. The time-resolved absorption was monitored during the process and quantitatively studied by fractal dimension and lacunarity analysis. The capability of nanoarchitecturing provides confirmation of complete monolayer formation and leads to tunable iridescent reflective colors of the MNP films. In addition, the MNP films have durable electrochemical conductivities as evidenced by enhanced charge storage capacities for 1000 cycles. Moreover, the MNP covered ITO (indium tin oxide) substrates significantly reduced secretion of inflammatory cytokines, TNF-α, by raw 264.7 macrophage cells compared to bare ITO, by a factor of 5 and 1.8 with and without lipopolysaccharide endotoxins, respectively. These results highlight the optoelectronic device-level tunability along with the anti-inflammatory biocompatibility of the MNP LBL film. This combination of performance should make these films particularly interesting for bioelectronic device applications such as electroceuticals, artificial bionic organs, biosensors, and implantable devices.

The reinforcement of polymer nanocomposites can be achieved through alignment or percolation of cellulose nanocrystals (CNCs). Here, we compare the efficacy of these reinforcement mechanisms in thermoplastic polyurethane (PU) elastomer nanocomposites containing thermally stable cotton CNCs. CNC alignment was achieved by melt spinning nanocomposite fibers, while a percolating CNC network was generated by solvent casting nanocomposite films with CNC contents up to 20 wt %. While in films both the CNCs and the PU matrix were entirely isotropic at all concentrations as confirmed by wide-angle X-ray scattering and birefringence analysis, the CNCs in the fibers exhibited a preferential orientation, which improved with increasing CNC concentration. Increasing the CNC concentration in the fibers reduces, however, the alignment of the PU chains, resulting in an entirely isotropic PU matrix at high CNC contents. The mechanical properties of films and fibers were evaluated using stress− strain measurements. Nanocomposite fibers with low CNC content exhibited superior stiffness, extensibility, and strength compared to the films, while the films displayed superior mechanical properties at high CNC concentrations. These findings are rationalized using common semiempirical models describing the reinforcing effects of CNC alignment in fibers (Halpin−Tsai) and CNC percolation in films (percolation model). The formation of a percolating CNC network leads to a stronger reinforcement than CNC alignment, as the reinforcing effect of the latter is limited by the comparably low aspect ratio of CNCs extracted from cotton. As a consequence, above the percolation threshold for cotton CNCs, isotropic nanocomposite PU films show a higher stiffness than aligned nanocomposite PU fibers.

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This paper highlights the influence of peptide secondary structure on the shape memory behaviour of peptidic polyureas, driven by hydrogen bonding arrangement and microphase-separated morphology.