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In nature, cellulose nanofibers form hierarchical structures across multiple length scales to achieve high-performance properties and different functionalities. Cellulose nanofibers, which are separated from plants or synthesized biologically, are being extensively investigated and processed into different materials owing to their good properties. The alignment of cellulose nanofibers is reported to significantly influence the performance of cellulose nanofiber-based materials. The alignment of cellulose nanofibers can bridge the nanoscale and macroscale, bringing enhanced nanoscale properties to high-performance macroscale materials. However, compared with extensive reviews on the alignment of cellulose nanocrystals, reviews focusing on cellulose nanofibers are seldom reported, possibly because of the challenge of aligning cellulose nanofibers. In this review, the alignment of cellulose nanofibers, including cellulose nanofibrils and bacterial cellulose, is extensively discussed from different aspects of the driving force, evaluation, strategies, properties, and applications. Future perspectives on challenges and opportunities in cellulose nanofiber alignment are also briefly highlighted.

The stiffness and tensile strength of biopolymers (e.g., polylactic acid (PLA)) are less than desirable for load-bearing applications in their neat form. The use of natural fibers as reinforcements...

The intrinsic brittleness of poly(lactic acid) (PLA) has hindered its widespread use in many structural applications. Various strategies have been developed to toughen PLA; however, most of the met...

Cellulose nanofibrils (CNFs) have been exploited for different applications, such as nanocomposites, gas separation, flexible electronics, and fuel cells, due to their unique properties. To fulfill...

Microfibrillated cellulose (MFC) is widely used as a reinforcement filler for biocomposites due to its unique properties. However, the challenge of drying MFC and the incompatibility between nanocellulose and polymer matrix still limits the mechanical performance of MFC-reinforced biocomposites. In this study, we used a water-based transesterification reaction to functionalize MFC and explored the capability of oven-dried MFC as a reinforcement filler for polylactic acid (PLA). Remarkably, this oven-dried, vinyl laurate-modified MFC improved the tensile strength by 38 % and Young's modulus by 71 % compared with neat PLA. Our results suggested improved compatibility and dispersion of the fibrils in PLA after modification. This study demonstrated that scalable water-based surface modification and subsequent straightforward oven drying could be a facile method for effectively drying cellulose nanomaterials. The method helps significantly disperse fibrils in polymers and enhances the mechanical properties of microfibrillar cellulose-reinforced biocomposites.

While PLA possesses modest to good strength and stiffness, broader application is hindered by its brittle nature. The aim of this study was to develop strong and tough polymeric materials from renewable biomaterials and understand the underlying interactions and mechanisms. Cellulose nanofibrils (CNFs) and epoxidized soybean oil (ESO) were compounded with poly(lactic acid) (PLA) to create a PLA-CNF-ESO tertiary nanocomposite system. Tensile and dynamic mechanical analyses were performed to see how variations in ESO and CNF content affect mechanical properties such as strength, modulus, ductility, and toughness. It was found that at low CNF levels (10 wt%) the addition of ESO can improve the ductility of the nanocomposites 5- to 10-fold with only slight losses in strength and modulus, while at higher CNF levels (20 and 30 wt%), ESO exhibited little effect on mechanical properties, possibly due to percolation of CNFs in the matrix, dominating stress transfer. Therefore, it is important to optimize CNF and ESO amounts in composites to achieve materials with both high strength and high toughness. Efforts have been made to understand the underlying mechanisms of the mechanical behavior of one class of these composites via thermal, dynamic mechanical, rheological, morphological, and Raman analyses.

Brittleness is a key barrier for poly(lactic acid) (PLA) toward broader applications. Supertough PLA was achieved by simply mixing a low amount (0.5–1 wt %) of organoalkoxysilane with PLA. Three organosilanes, (3-aminopropyl)triethoxysilane (APTES), 3-(triethoxysilyl)propyl isocyanate (ICPTES), and trimethoxymethylsilane (MTMS), were selected for this study to understand how the functional group on a silane affects the behavior of the PLA-silane hybrids. Remarkable improvements in ultimate tensile strain (up to 12 folds) and tensile toughness (up to 10 folds) were observed in APTES- and ICPTES-modified PLA without any loss in tensile strength and modulus. Glass transition temperatures measured by differential scanning calorimetry (DSC) and dynamic mechanical analysis (DMA) did not show any obvious decrease. We propose that in situ condensation of organosilane and grafting of PLA to form a silica-PLA core–shell nanocomplex may be the reason for the improved mechanical properties. Scanning electron microsco...

Advanced templating techniques have enabled delicate control of both nano- and microscale structures and have helped thrust functional materials into the forefront of society. Cellulose nanomaterials are derived from natural polymers and show promise as a templating source for advanced materials. Use of cellulose nanomaterials in templating combines nanoscale property control with sustainability, an attribute often lacking in other templating techniques. Use of cellulose nanofibers for templating has shown great promise in recent years, but previous reviews on cellulose nanomaterial templating techniques have not provided extensive analysis of cellulose nanofiber templating. Cellulose nanofibers display several unique properties, including mechanical strength, porosity, high water retention, high surface functionality, and an entangled fibrous network, all of which can dictate distinctive aspects in the final templated materials. Many applications exploit the unique aspects of templating with cellulose nanofibers that help control the final properties of the material, including, but not limited to, applications in catalysis, batteries, supercapacitors, electrodes, building materials, biomaterials, and membranes. A detailed analysis on the use of cellulose nanofibers templating is provided, addressing specifically how careful selection of templating mechanisms and methodologies, combined toward goal applications, can be used to directly benefit chosen applications in advanced functional materials.

Cellulose nanocrystal (CNC)-based composite films were prepared as a solid electrolyte for alkaline fuel cells. Poly(vinyl alcohol) (PVA) and silica gel hybrid were used to bind the CNCs to form a robust composite film. The mass ratio (i.e., 1 : 1, 1 : 2) of PVA and silica gel was tuned to control the hydrophobicity of the resulting films. Composite films with a range of CNC contents (i.e., 20–60%) were prepared to demonstrate the impact of CNCs on the performance of these materials as a solid electrolyte for alkaline fuel cells. Different from previously reported cross-linked polymer films, CNC-based composite films with 40% hydrophobic binder (i.e., PVA : silica gel = 1 : 2) exhibited simultaneous low water swelling (e.g., ∼5%) and high water uptake (e.g., ∼80%) due to the hydrophilicity and extraordinary dimensional stability of CNCs. It also showed a conductivity of 0.044 and 0.065 S cm−1 at 20 and 60 °C, respectively. To the best of our knowledge, the film with 60% CNC and 40% binder is characterized by the lowest hydroxide conductivity-normalized swelling ratio. Decreased CNC contents (i.e., 40 and 20%) resulted in comparable hydroxide conductivity but a greater swelling ratio. These results demonstrate the advantage of CNCs as a key component for a solid electrolyte for alkaline fuel cells over conventional polymers, suggesting the great potential of CNCs in improving the dimensional stability while maintaining the conductivity of existing anion exchange membranes.

ORNL worked with American Process Inc. to demonstrate the potential use of bio-based BioPlus® lignin-coated cellulose nanofibrils (L-CNF) as a reinforcing agent in the development of polymer feedstock suitable for additive manufacturing. L-CNF-reinforced polylactic acid (PLA) testing coupons were prepared and up to 69% increase in tensile strength and 133% increase in elastic modulus were demonstrated.

Palladium-doped activated carbon fibers are being evaluated as candidate materials for enhanced hydrogen storage at near ambient conditions. Pd-doped fibers were spun using a Pd salt mixed with an isotropic pitch precursor. Experimental techniques such as in situ X-ray analysis, thermogravimetric studies, scanning transmission electron microscopy and gas adsorption were employed to understand how processing conditions for the production of Pd-doped activated carbon fibers affect the microstructure, pore development, and dispersion of metal particles throughout the fibers. The results showed that PdO phase is present in the stabilized fibers and that this oxide phase is stable up to about 250 °C. The oxide phase transforms into Pd metal with increasing heat treatment temperature, going through the formation of an intermediate carbide phase. Sintering of Pd particles was observed with heat treatment at temperatures over 750 °C. It was also found that pore development during physical activation with CO2 was not significantly affected by the presence of Pd particles within the fibers.