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Highlights • Evaluation of LPMO activity on cellulosic substrates of different crystallinity. • SamLPMO10C is more active on celluloses with high crystallinity and accessibility. • Synergism of LPMOs and endoglucanases on NFC production from flax. • First study reporting the effect of a bacterial LPMO in nanocellulose production. Abstract A series of cellulosic substrates has been produced, treated with lytic polysaccharide monooxygenase (LPMO) from Streptomyces ambofaciens (SamLPMO10C), and analyzed by high performance anion exchange chromatography (HPAEC) with pulsed amperometric detection (PAD). The activity of the bacterial LPMO showed high variability depending on the origin and degree of crystallinity of the substrate. Additionally, we tested the effectiveness of SamLPMO10C in the nanofibrillation of flax, a high crystalline agricultural fiber, as a single pretreatment or in combination with cellulases. All pretreatments were followed by a mechanical defibrillation by high-pressure homogenization (HPH) to obtain cellulose nanofibrils (NFC). The combined LPMO-cellulase treatment showed higher fibrillation yield, optical transmittance and carboxylate content than control reactions. Therefore, it could be explored as a promising green alternative to reduce the energy consumption in the production of NFC. To our knowledge, this is the first study reporting the effect of a bacterial LPMO in nanocellulose production. [ABSTRACT FROM AUTHOR]

Bioinspiration from hierarchical structures found in natural environments has heralded a new age of advanced functional materials. Nanocellulose has received significant attention due to the demand for high-performance materials with tailored mechanical, physical and biological properties. In this study, nanocellulose fibrils, nanocrystals and a novel mixture of fibrils and nanocrystals (blend) were prepared from softwood biomass using the AVAP® biorefinery technology. These materials were characterized using transmission and scanning electron microscopy, and atomic force microscopy. This analysis revealed a nano- and microarchitecture with extensive porosity. Notable differences included the nanocrystals exhibiting a compact packing of nanorods with reduced porosity. The NC blend exhibited porous fibrillar networks with interconnecting compact nanorods. Fourier transform infrared spectroscopy and X-ray diffraction confirmed a pure cellulose I structure. Thermal studies highlighted the excellent stability of all three NC materials with the nanocrystals having the highest decomposition temperature. Surface charge analysis revealed stable colloid suspensions. Rheological studies highlighted a dominance of elasticity in all variants, with the NC blend being more rigid than the NC fibrils and nanocrystals, indicating a double network hydrogel structure. Given these properties, it is thought that these materials show great potential in (bio)nanomaterial applications where careful control of microarchitecture, surface topography and porosity are required. [ABSTRACT FROM AUTHOR]

Development of strong cellulose nanofibril (CNF) networks for advanced applications, such as in the biomedical field, is of high importance owing to the biocompatible nature and plant-based origin of cellulose nanofibrils. Nevertheless, lack of mechanical strength and complex synthesis methods hinder the application of these materials in areas where both toughness and manufacturing simplicity are required. In this work, we introduce a facile method for the synthesis of a low solid content (< 2 wt%), covalently crosslinked CNF hydrogel where Poly (N-isopropylacrylamide) (NIPAM) chains are utilized as crosslinks between the nanofibrils. The resulting networks have the capability to fully recover the shape in which they were formed after various drying and rewetting cycles. Characterization of the hydrogel and its constitutive components was performed using X-ray scattering, rheological investigations and uniaxial testing in compression. Influence of covalent crosslinks was compared with networks crosslinked by the addition of CaCl 2. Among other things the results show that the mechanical properties of the hydrogels can be tuned by controlling the ionic strength of the surrounding medium. Finally, a mathematical model was developed based on the experimental results, which describes and predicts to a decent degree the large-deformation, elastoplastic behavior, and fracture of these networks. [Display omitted] [ABSTRACT FROM AUTHOR]

A hybrid catalyst was prepared using cellulose nanofibrils and magnetite to degrade organic compounds. Cellulose nanofibrils were isolated by mechanical defibrillation producing a suspension used as a matrix for magnetite particles. The solution of nanofibrils and magnetite was dried and milled resulting in a catalyst with a 1:1 ratio of cellulose and magnetite that was chemically and physically characterized using light, scanning electron and transmission electron microscopies, specific surface area analysis, vibrating sample magnetometry, thermogravimetric analysis, Fourier transform infrared spectroscopy, X-ray diffraction, catalytic potential and degradation kinetics. Results showed good dispersion of the active phase, magnetite, in the mat of cellulosic nanofibrils. Leaching and re-use tests showed that catalytic activity was not lost over several cycles. The hybrid material produced was tested for degradation of methylene blue dye in Fenton-like reactions resulting in a potential catalyst for use in degradation of organic compounds. [ABSTRACT FROM AUTHOR]

Fabricating alginate fibers of high strength and toughness remains a great challenge because of the difficulty in improving both strength and toughness simultaneously. Herein, this work reported the hierarchical assembly of sodium alginate nano-helix and its potential application as a new reinforcing unit for alginate fibers. Contributed from the hierarchical structures of α-helix, β-sheet and tertiary helical alignment of nanofibrils, nano-helix improved the tensile strength of fibers with enhanced modulus, and prolonged elongation through unravelling the tertiary structures. Thus, the strength, elongation and toughness of alginate fibers were all enhanced by >200 %, solving the tradeoff of strength and toughness. The mechanical performance of nano-helix engineered alginate fibers is superior to present alginate fibers and even some other biomass-based fibers. The assembly of nano-helix provides a feasible reinforcing strategy for polysaccharide based materials, achieving simultaneous improvement of strength and toughness. [Display omitted] • Hierarchical nano-helix is composed of α-helix, β-sheet and tertiary structure of helical alignment of nanofibrils. • Hierarchical nano-helix is prepared through three stages of assembly with reorganized secondary structures. • Hierarchical nano-helix is a structural reinforcing unit for simultaneous improvement of strength and toughness. [ABSTRACT FROM AUTHOR]

Present study illustrates the preparation of chitin nanofibrils (CNF) reinforced carrageenan nanocomposite films by the solution-casting technique. CNF was prepared by acid hydrolysis of chitin, followed by high speed homogenization and sonication. FTIR result demonstrated that the chemical structure of chitin had not changed after acid hydrolysis. However, the crystalinity of CNF was found to be higher than chitin. The crystallite size of chitin and CNF was 4.73 and 6.27 nm, respectively. The char content at 600 °C of chitin (19.2%) was lower than the CNF (25%). The carrageenan/CNF composite films were smooth and flexible and the CNF was dispersed uniformly in the carrageenan polymer matrix. The tensile strength and modulus of carrageenan film were increased significantly ( p < 0.05) after CNF reinforcement with up to 5 wt%, however, elongation at break, water vapor permeability, and transparency decreased slightly. Carrageenan/CNF nanocomposite films showed strong antibacterial activity against a Gram-positive food-borne pathogen, Listeria monocytogenes. [ABSTRACT FROM AUTHOR]

Carbohydrate-based nanofibrils, including cellulose nanofibrils (CNFs) and chitin nanofibrils (ChNFs) are highly ordered architectures which are the basis of various biological components with hierarchical features, low-cost, biocompatibility, and biofunctionality. To preserve these exceptional structural topographies and to directly use these natural nanofibrils assembly, different approaches have been introduced to exfoliate these nanofibrils from their origin. In this review, we aim to summarize the recent progress on the isolation methods of CNFs and ChNFs and their relation to their physical and chemical properties. In addition, recent studies on their biomedical applications, focusing on tissue engineering, wound dressing, biomedical implants, drug delivery, and biosensors are emphasized. After short evaluation of the toxicity and immunogenicity of these nanofibrils, the outlooks and current challenges of CNFs and ChNFs-based constructs for biomedical applications are summarized. This study shows that CNFs and ChNFs-based constructs have significant potential for a widespread biomedical application in the future. [Display omitted] • Diverse nanofibrillls for tissue engineering are introduced. • The extraction methods of the nanofibrils, along with their advantages and disadvantages are reviewed. • The physical and mechanical properties of diverse nanofibrils are presented. • The latest development of nanofibrils for tissue engineering applications is presented. [ABSTRACT FROM AUTHOR]

Abstract: There is growing interest in cellulose nanofibres from renewable sources for several industrial applications. However, there is a lack of information about one of the most abundant cellulose pulps: bleached Eucalyptus kraft pulp. The objective of the present work was to obtain Eucalyptus cellulose micro/nanofibres by three different processes, namely: refining, sonication and acid hydrolysis of the cellulose pulp. The refining was limited by the low efficiency of isolated nanofibrils, while sonication was more effective for this purpose. However, the latter process occurred at the expense of considerable damage to the cellulose structure. The whiskers obtained by acid hydrolysis resulted in nanostructures with lower diameter and length, and high crystallinity. Increasing hydrolysis reaction time led to narrower and shorter whiskers, but increased the crystallinity index. The present work contributes to the different widespread methods used for the production of micro/nanofibres for different applications. [Copyright &y& Elsevier]

The objective of this research is to develop a functional medical adhesive from natural nanofibril-stabilized latex through an aqueous process. Surface charged cellulose or chitin nanofibrils are used to form Pickering emulsions of acrylic monomers, followed by in situ polymerization. Charged initiators are selected to tailor the interactions between them and nanofibrils, and it is found that the repulsive electrostatic interactions play a key role in stabilizing the heterogeneous system. As a result, poly(2-ethylhexyl acrylate- co -methyl methacrylate) latexes are successfully prepared for surfactant-free adhesives with a high shear strength of 72.0 ± 6.5 kPa. In addition, drug can be easily incorporated in the nanopaper substrate or adhesive layer to form a medical tape, exhibiting long-term drug release and antibacterial behaviors. We managed developing a facile method to integrate green synthesis, versatile functionalities and excellent adhesion into one adhesive, which remains a great challenge. [Display omitted] [ABSTRACT FROM AUTHOR]

A high-yield and straightforward method is proposed to obtain an electromagnetic interference (EMI) shielding film based on multilayered Ti 3 C 2 T x (m-Ti 3 C 2 T x). Holocellulose nanofibrils modified by sulfamic acid (SHCNF) with unique "core-shell" structure can act as a dispersant and a binder to assist in exfoliating m-Ti 3 C 2 T x into delaminated-Ti 3 C 2 T x (d-Ti 3 C 2 T x) and fabricate flexible Ti 3 C 2 T x /SHCNF composite films with a high-yield value. The "brick-and-mortar" composite films exhibit a superior electromagnetic interference (EMI) shielding effectiveness (SE) of 45.02 dB with an ultrathin thickness of 40 μm at the 12.4 GHz. Moreover, these flexible and strong integrated Ti 3 C 2 T x /SHCNF composite films also display excellent specific EMI SE of SSE/t (4437 dB cm2 g−1) and high EMI shielding efficiency (99.996%). Therefore, the SHCNF-assisted method provides a cost-effective approach to fabricate a strong and flexible MXene-based nanocomposite films toward EMI shielding application. [Display omitted] • Holocellulose nanofibrils assisted in exfoliating multilayered Ti 3 C 2 T x. • The Ti 3 C 2 T x /SHCNF film exhibited superior mechanical properties. • The film presented excellent specific EMI shielding efficiency. [ABSTRACT FROM AUTHOR]

Commercializing dried microfibrillated cellulose (MFC) has always been a challenge mainly due to the tendency of MFC to aggregate. In this study MFC samples were submitted to drying/redispersion cycles at different temperatures. Morphology, crystallinity and mechanical performance of films were analyzed throughout the cycles. Microscopy images, particle size and stability in water showed that aggregation happens more severely with 5 drying/redispersion cycles and at drying temperatures of 75 and 100 °C. Particles once-dried at 20 °C formed the same size and web-like structure as the MFC-control. Crystallinity and crystallite sizes increased with drying/redispersion cycles especially when dried at 75 and 100 °C, however drying/redispersion cycles also led to a reduction in mechanical performance due to aggregation. While oven-drying is not the most suitable method, milder action at room temperature once-drying led to suspension stability in water, morphology and mechanical properties close to never-dried MFC, which makes this treatment a feasible option to maintain cellulose quality. [ABSTRACT FROM AUTHOR]