Melt processing of polyamide 12 and cellulose nanocrystals nanocomposites

The fabrication of nanocomposites of polyamide 12 (PA12) and cellulose nanocrystals (CNCs) isolated from cotton and tunicates is reported. Through a comparative study that involved solution‐cast (SC) and melt‐processed materials, it was shown that PA12/CNC nanocomposites can be prepared in a process that appears to be readily scalable to an industrial level. The results demonstrate that CNCs isolated from the biomass by phosphoric acid hydrolysis display both a sufficiently high thermal stability to permit melt processing with PA12, and a high compatibility with this polymer to allow the formation of nanocomposites in which the CNCs are well dispersed. Thus, PA12/CNC nanocomposites prepared by melt‐mixing the two components in a co‐rotating roller blade mixer and subsequent compression molding display mechanical properties that are comparable to those of SC reference materials. Young's modulus and maximum stress could be doubled in comparison to the neat PA12 by introduction of 10% (CNCs from tunicates) or 15% w/w (CNCs from cotton) CNCs. © 2015 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2015 , 132, 42752.     

Cellulose nanocrystal‐based poly(butylene adipate‐co‐terephthalate) nanocomposites covered with antimicrobial silver thin films

In this study, we reported the preparation and prospective application of the nanocomposites of poly(butylene adipate‐co‐terephthalate) (PBAT) reinforced with cellulose nanocrystals (CNCs). CNCs were isolated from bleached sugarcane bagasse by acid hydrolysis and functionalized with adipic acid. Nanocomposites were prepared with different concentration of CNCs (0.8, 1.5, and 2.3 wt% CNC) by solution‐casting method and then were covered with silver thin film by magnetron sputtering. The results showed that the surface modification increased the degree of crystallinity of nanocrystals from 51% to 56%, decreasing their length and diameter. Moreover, AFM‐IR spectroscopy revealed that the modified CNCs were covered by adipic acid molecules, improving the dispersion of nanocrystals in PBAT. Well‐dispersed modified CNCs acted as heterogeneous nuclei for crystallization of PBAT, and increased the storage modulus of the polymer by more than 200%. These improvements in thermal and mechanical properties of CNC‐based PBAT associated with the decrease of 56% in the Escherichia coli biofilm formation on nanocomposites (antibacterial properties) qualify the CNC/PBAT nanocomposites covered with silver thin films to be used as food packaging. POLYM. ENG. SCI., 59:E356–E365, 2019. © 2019 Society of Plastics Engineers     

Poly(methyl methacrylate)‐grafted cellulose nanocrystals: One‐step synthesis,nanocomposite preparation,and characterization

Cellulose nanocrystals (CNCs) are ideal reinforcing agents for polymer nanocomposites because they are lightweight and nano‐sized with a large aspect ratio and high elastic modulus. To overcome the poor compatibility of hydrophilic CNCs in non‐polar composite matrices, we grafted poly(methyl methacrylate) (PMMA) from the surface of CNCs using an aqueous, one‐pot, free radical polymerization method with ceric ammonium nitrate as the initiator. The hybrid nanoparticles were characterized by CP/MAS NMR, X‐ray photoelectron spectroscopy, infrared spectroscopy, contact angle, thermogravimetric analysis, X‐ray diffraction, and atomic force microscopy. Spectroscopy demonstrates that 0.11 g/g (11 wt %) PMMA is grafted from the CNC surface, giving PMMA‐g‐CNCs, which are similar in size and crystallinity to unmodified CNCs but have an onset of thermal degradation 45 °C lower. Nanocomposites were prepared by compounding unmodified CNCs and PMMA‐g‐CNCs (0.0025–0.02 g/g (0.25–2 wt %) loading) with PMMA using melt mixing and wet ball milling. CNCs improved the performance of melt‐mixed nanocomposites at 0.02 g/g (2 wt %) loading compared to the PMMA control, while lower loadings of CNCs and all loadings of PMMA‐g‐CNCs did not. The difference in Young's modulus between unmodified CNC and polymer‐grafted CNC composites was generally insignificant. Overall, ball‐milled composites had inferior mechanical and rheological properties compared to melt‐mixed composites. Scanning electron microscopy showed aggregation in the samples with CNCs, but more pronounced aggregation with PMMA‐g‐CNCs. Despite improving interfacial compatibility between the nanoparticles and the matrix, the effect of PMMA‐g‐CNC aggregation and decreased thermal stability dominated the composite performance.     

Cellulose nanocrystal driven crystallization of poly(d,l‐lactide) and improvement of the thermomechanical properties

The technological exploitation of polylactide in fields requiring wide range of operating conditions is limited by the low crystallization rate of the polymer and therewith the low thermomechanical stability. Here we report the crystallization and consequent improvement of the thermomechanical properties of originally amorphous poly(d,l ‐lactide) (d : l ratio 11 : 89) loaded with cellulose nanocrystals (CNCs). Isothermal treatment of samples with different CNC contents and at various temperatures, showed up to 6 wt % crystalline phase formation, as confirmed by differential scanning calorimetry and X‐ray diffraction measurements. Under a particular set of annealing conditions, CNCs promote the formation of a lamellar structure. This provides the system with higher order and cohesion which in combination with stress‐transfer between CNCs, led to an increase of the storage modulus in the rubbery plateau up to 30 times (from 2.7 MPa up to 79 MPa), a rise of the melting temperature up to 50°C, and an improvement of the Young's modulus up to 40%. © 2014 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2015 , 132, 41607.     

Development and characterization of bionanocomposites based on poly(3‐hydroxybutyrate) and cellulose nanocrystals for packaging applications

Poly(3‐hydroxybutyrate) (PHB)‐based bionanocomposites were prepared using various percentages of cellulose nanocrystals (CNCs) by a solution casting method. CNCs were prepared from microcrystalline cellulose using sulfuric acid hydrolysis. The influence of CNCs on PHB properties was evaluated using differential scanning calorimetry, Fourier transform infrared spectroscopy, X‐ray diffraction, thermogravimetry and tensile testing. Vapor permeation and light transmission of the materials were also measured. Differential scanning calorimetric tests demonstrated that CNCs were effective PHB nucleation agents. Tensile strength and Young's modulus of PHB increased with increasing CNC concentration. Moreover, the PHB/CNC bionanocomposites exhibited reduced water vapor permeation compared to neat PHB and had better UV barrier properties than commodity polymers such as polypropylene. It was found that nanocomposites with 6 wt% of CNCs had the optimum balance among thermal, mechanical and barrier properties. © 2016 Society of Chemical Industry     

Increased thermal stability of nanocellulose composites by functionalization of the sulfate groups on cellulose nanocrystals with azetidinium ions

Cellulose nanocrystals (CNCs) prepared via sulfuric acid hydrolysis are decorated with sulfate groups that yield a stable water suspension. To make the CNCs adaptable for use in composites, the hydroxyl groups on the surface are usually hydrophobized. In this article, an alternative hydrophobization method is described in which the sulfate groups are conjugated with azetidinium salts. The results of this study show that the sulfate groups can be functionalized with azetidinium salts and from thermal studies, it was discovered that the functionalization led to a 100 °C increase in thermal stability, compared with unmodified CNCs. The nanocomposites prepared by extrusion of CNC‐coated low‐density polyethylene powder displayed similar mechanical properties as the CNC‐reference sample, but without the discoloration, due to the increased thermal stability. In conclusion, the azetidinium reagent reacts preferentially with sulfate groups, and this new type of chemical conversion of sulfate groups on polysaccharides will be beneficial in nanocomposite manufacturing. © 2017 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2018 , 135, 45963.     

Functionally Graded Polyurethane/Cellulose Nanocrystal Composites

The preparation and investigation of functionally graded polymer nanocomposites, which have a concentration gradient of cellulose nanocrystals (CNCs) along one direction, is reported here. As a test bed, a series of nanocomposites consisting of a thermoplastic polyurethane (PU) and 0–15% w/w CNCs is prepared via solvent casting and the mechanical properties of films of these materials are characterized by dynamic mechanical analyses and tensile tests. The formation of graded materials is accomplished by lamination of films with varying CNC content. The processing conditions are optimized to achieve intimate fusion of the individual layers. The elimination of internal interfaces is evidenced by an elongation at break of up to 500%. In order to explore potential applications of graded PU/CNC nanocomposites, structure‐dependent actuation in response to water is demonstrated in a bioinspired architecture. In addition, the damping behavior of cylindrical shaped composites is investigated by way of compression tests. The results show that functionally graded PU/CNC composites show good damping behavior over a much larger range of forces than the neat PU or the homogeneous nanocomposites.     

Cellulose acetate ultrafiltration membranes reinforced by cellulose nanocrystals: Preparation and characterization

Cellulose nanocrystals (CNCs) were used as a sustainable additive to improve the hydrophilicity, permeability, antifouling, and mechanical properties of blend membranes. Different CNC loadings (0–1.2 wt %) in cellulose acetate (CA) membranes were studied. The blend membranes were prepared by a phase‐inversion process, and their chemical structure and morphological properties were characterized by attenuated total reflectance–Fourier transform infrared spectroscopy, scanning electron microscopy, porosity, and mean pore size and contact angle measurement. The blend membranes became more porous and more interconnected after the addition of CNCs. The thickness of the top layer decreased and a few large holes in the porous substrate appeared with increasing CNC loading. In comparison with the pure CA membranes, the pure water flux of the blend membranes increased with increasing CNC loading. It reaches a maximum value of 76 L m^?2 h^?1 when the CNC loading was 0.5 wt %. The antifouling properties of the CA membrane were significantly improved after the addition of CNCs, and the flux recovery ratio value increased to 68% with the addition of 0.5 wt % CNCs. In comparison with that of the pure CA membranes, the tensile strength of the composite membranes increased by 47%. This study demonstrated the importance of using sustainable CNCs to achieve great improvements in the physical and chemical performance of CA ultrafiltration membranes and provided an efficient method for preparing high‐performance membranes. © 2016 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2016 , 133, 43946.     

Surface modification and antimicrobial properties of cellulose nanocrystals

A novel and simple surface modification of cellulose nanocrystals (CNC) was performed by chloroacetylation and subsequent reaction with tertiary amines to form quaternary ammonium modified CNCs. The acetylation of CNC and quaternary ammonium modified CNCs was confirmed using IR spectroscopy and solid state NMR spectroscopy. The ¹³C NMR spectrum of quaternary ammonium modified CNC showed several additional resonances ranging from 14.5 ppm to 58.0 ppm compared to ¹³C NMR spectrum of pure CNC, suggesting that alkyl chains have been added to the pure CNC. The disc diffusion method was used to evaluate the antimicrobial properties of quaternary ammonium modified CNCs. It was found that modified CNCs with alkyl chain longer than ten carbons are effective antimicrobial agents against Staphylococcus aureus and E. coli bacteria. These CNCs can be chemically modified to tailor the properties to improve dispersion in the polymer matrix. This will expand the application of CNC as a reinforcing material. © 2017 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2017 , 134, 44789.     

Reinterpretation of the mechanical reinforcement of polymer nanocomposites reinforced with cellulose nanorods

The mechanical reinforcement of nanocomposites containing nanorods‐like fillers such as cellulose nanocrystals (CNCs) is often interpreted by adapting the classical parallel–series model, assuming a simple hyperbolic dependence between the percolation threshold and aspect ratio. However, such assumptions are valid only for nanorods with high aspect ratio and often are misinterpreting the reinforcement obtained at low volume fraction of filler loading. To elucidate this intriguing scenario, we proposed a new approach and validated it by compiling and reinterpreting some of available literature that represent the experimental reinforcement with CNCs. Our approach showed better accuracy, specifically for the cases of CNC nanorods with lower aspect ratio. We conclude that this route permits a more realistic evaluation of the mechanical reinforcement, where a physical parameter accounting the polymer filler association is introduced. © 2017 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2017 , 134, 45254.     

Polyamide 6 nanocomposites incorporating cellulose nanocrystals prepared by In situ ring‐opening polymerization: Viscoelasticity,creep behavior,and melt rheological properties

The creep behavior and solid and melt linear viscoelasticity of novel polyamide 6 (PA6) nanocomposites reinforced with cellulose nanocrystals (CNCs) prepared via in situ anionic ring‐opening polymerization (ROP) were investigated to accelerate research efforts to develop new polymeric materials with improved properties for lightweight, load‐bearing applications. The obtained results showed that incorporation of relatively small amounts of ≤ 2wt% CNCs into the PA6 thermoplastic matrix gave nanocomposite samples with significantly enhanced creep and viscoelastic materials functions of the PA6 as indicated by lower creep strain, lower creep compliance, improved elastic recovery after removal of load, and reduced Arrhenius activation energies for time‐dependent viscoplastic flow. The obtained results were analyzed and interpreted by theoretical equations for predicting the viscoelasticity and creep behavior of polymeric systems. The melt rheological properties showed enhanced melt strength and elasticity. The formation of a percolated network structure of CNC was revealed by morphological observations that were consistent with the dynamic structure break‐up and reformation rheological experiments. The stiffness, rigidity of the CNCs along with their special ROP‐facilitated intrinsic strong chemical interactions with the PA6 matrix is believed to be responsible for the observed superior creep and viscoelastic materials functions even with very little CNC concentration. POLYM. ENG. SCI. 56:1045–1060, 2016. © 2016 Society of Plastics Engineers     

Preparation and characterization of polybutylene‐succinate/poly(ethylene‐glycol)/cellulose nanocrystals ternary composites

Ternary composites were prepared by twin screw extrusion from polybutylene‐succinate (PBS), poly(ethylene‐glycol) (PEG), and cellulose nanocrystals (CNC). The aim of the work is to improve the physical–mechanical properties of PBS by the addition of CNC. A PEG/CNC masterbatch was prepared in order to achieve a good dispersion of hydrophilic CNC in the hydrophobic PBS. The influence of the nanoparticle content on the polymer properties was studied. Regarding the thermal properties fractioned crystallization phenomena of PEG was observed during cooling from the melt. No significant nucleating effect of the nanocellulose was observed. The material containing 4 wt % of CNC showed the best mechanical performance among the nanocomposites studied due to the combination of high modulus and elongation at break with a low detrimental in strength compared with the PBS/PEG blend. Moreover, no nanocellulose agglomerations were observed in its FESEM micrograph. © 2015 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2016 , 133, 43302.     

Preparation and characterization of poly(glycerol sebacate)/cellulose nanocrystals elastomeric composites

Poly(glycerol sebacate) (PGS) is one of the new elastomers used for soft tissue engineering, while improving its limited mechanical strength is the biggest challenge. In this work, a novel biodegradable elastomer composite PGS/cellulose nanocrystals (CNCs) was prepared by solution‐casting method and the mechanical properties, sol–gel contents, crosslink density, and hydrophilic performance were characterized. The thermal and degradation properties of composites were also investigated. Results show that the addition of CNCs into PGS resulted a significant improvement in tensile strength and modulus, as well as the crosslink density and the hydrophilicity of PGS. When the CNCs loading reached 4 wt %, the tensile strength and modulus of the composite reached 1.5 MPa and 1.9 MPa, respectively, resulting 204% and 158% increase compared to the pure PGS. Prolonging the curing time also improved the strength of both the neat PGS and PGS/CNCs composites according to the association and shift of hydroxy peaks around 3480 cm^?1. DSC results indicate that the addition of CNCs improved both the crystallization capacity and moving capability of PGS molecular chain. © 2015 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2015 , 132, 42196.     

Analyzing three‐dimensional structure and geometrical shape of individual cellulose nanocrystal from switchgrass

The three‐dimensional morphology, size distribution, and structure of individual cellulose nanocrystals (CNCs) isolated from switchgrass (Panicumvirgatum L), a representative raw biomass material, were investigated in this research. Width and height evolutions along the individual CNC longitudinal direction were statistically and quantitatively characterized using transmission electron microscopy (TEM) and atomic force microscopy (AFM). Lognormal distribution was identified as the most likely for cellulose nanocrystals’ size distribution. Height and width dimensions were shown to decrease toward the ends from the midpoint of individual CNCs, implying a spindle shape. The observed rough surfaces of CNCs were explainable as the results of acid etching of the subcrystalline and disordered region located at the surface. X‐ray diffraction analysis of crystallite size accompanied with TEM and AFM measurements revealed that the cross‐sectional dimensions of individual switchgrass CNC were either rectangularly or elliptically shaped, with an approximately 3–5 nm lateral element length range. POLYM. COMPOS., 38:2368–2377, 2017. © 2015 Society of Plastics Engineers     

Enhanced thermal stability of biomedical thermoplastic polyurethane with the addition of cellulose nanocrystals

Freeze‐dried cellulose nanocrystals (CNCs) were dispersed in the thermoplastic polyurethane [Pellethane 2363‐55D (P55D)] by a solvent casting method to fabricate CNC‐reinforced nanocomposites. This study demonstrated that the addition of small amounts (1–5 wt %) of CNCs to P55D increased the thermal degradation temperature while maintaining a similar stiffness, strength, and elongation of the neat P55D. CNC additions to P55D did not alter the glass‐transition temperature, but the onset decomposition temperature was shifted from 286 to 327°C when 1 wt % CNCs was dispersed in the matrix. The higher onset decomposition temperature was attributed to the formation of hydrogen bonds between the hydroxyl groups on the CNC surface and urethane groups in the hard block of P55D. The ultimate tensile strength and strain to failure (ε_f) of the nanocomposites were minimally affected by additions up to 5 wt % CNCs, whereas the elastic modulus was increased by about 70%. The observation that ε_f was unchanged with the addition of up to 5 wt % CNCs suggested that the flow/sliding of the hard blocks and chains were not hindered by the presence of the CNCs during plastic deformation. The ramifications of this study was that CNC additions resulted in wider processing temperatures of P55D for various biomedical devices while maintaining a similar stiffness, strength, and elongation. © 2015 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2015 , 132, 41970.     

Melt extruded nanocomposites of polybutylene adipate‐co‐terephthalate (PBAT) with phenylbutyl isocyanate modified cellulose nanocrystals

Traditional commodity polymers are widely used in several disposable or short‐life items and take hundreds of years to decompose in nature. These polymers could be replaced in several uses by biodegradable polymers, like polybutylene adipate‐co‐terephthalate (PBAT) studied in this work. For this, nonetheless, it is necessary to improve some of the PBAT properties, like mechanical resistance and barrier properties. In this work, cellulose nanocrystals (CNC) were incorporated in PBAT with this intention, through melt extrusion. Aiming to avoid CNC aggregation during the drying and extrusion process, a CNC chemical modification with phenylbutyl isocyanate was done. It was possible to obtain PBAT‐CNC melt extruded composites with an elastic modulus 55% higher and water vapor permeability 63% lower than the values of the pure polymer, without compromising PBAT biodegradation. Therefore, the composites prepared with these enhanced properties have great potential as substitutes for traditional commodity polymers. © 2016 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2016 , 133, 43678.     

Bio‐nanocomposite films based on cellulose nanocrystals filled polyvinyl alcohol/chitosan polymer blend

Bio‐nanocomposite films based on polyvinyl alcohol/chitosan (PVA/CS) polymeric blend and cellulose nanocrystals (CNC) were prepared by casting a homogenous and stable aqueous mixture of the three components. CNC used as nanoreinforcing agents were extracted at the nanometric scale from sugarcane bagasse via sulfuric acid hydrolysis; then they were characterized and successfully dispersed into a PVA/CS (50/50, w/w) blend to produce PVA/CS–CNC bio‐nanocomposite films at different CNC contents (0.5, 2.5, 5 wt %). Viscosity measurement of the film‐forming solutions and structural and morphological characterizations of the solid films showed that the CNC are well dispersed into PVA/CS blend forming strong interfacial interactions that provide an enhanced load transfer between polymer chains and CNC, thus improving their properties. The obtained bio‐nanocomposite films are mechanically strong and exhibit improved thermal properties. The addition of 5 wt % CNC within a PVA/CS blend increased the Young's modulus by 105%, the tensile strength by 77%, and the toughness by 68%. Herein, the utilization of Moroccan sugarcane bagasse as raw material to produce high quality CNC has been explored. Additionally, the ability of the as‐isolated CNC to reinforce polymer blends was studied, resulting in the production of the aforementioned bio‐nanocomposite films with improved properties. © 2015 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2015 , 132, 42004.     

Modified cellulose nanocrystals enhancement to mechanical properties and water resistance of vegetable oil-based waterborne polyurethane

Environmentally friendly and lightweight silylated cellulose nanocrystal (SCNCs)/waterborne polyurethane (WPU) composite films that exhibit excellent mechanical properties and water resistance were prepared. The cellulose nanocrystals (CNCs) of the filamentous structure were surface-modified by γ-aminopropyltriethoxysilane (APTES) and then introduced into a castor oil-based aqueous polyurethane (WPU) matrix by in situ polymerization. The morphology and silylation degree of CNCs were characterized by scanning electron microscopy (SEM), thermogravimetric analysis (TGA), and Fourier infrared transform spectroscopy at different APTES concentrations. The results showed that the surface of the nanocellulose crystal has the best silylation morphology and thermal stability with incorporation of 6 wt % APTES. The thermal stability, mechanical properties, surface morphology, and water resistance of the nanocomposites were investigated by TGA, tensile test, SEM and optical contact angle, water absorption test, and mechanical property test after immersed in water. It was found that the effective introduction of modified CNCs resulted in a significant increase in tensile strength at high levels, and the thermal stability and hydrophobicity of the material were improved simultaneously, reaching the percolation threshold at a 0.50 wt % SCNCs as determined theoretically. This study provided an approach to the design and development of surface-modified CNCs/vegetable oil-based polymer composites by using an appropriate concentration of silane coupling agent to modify CNCs and improve the compatibility between nanocellulose and vegetable oil-based polymer matrices. © 2019 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2019 , 136, 48228.     

Characterization and mechanical properties of ultraviolet stimuli‐responsive functionalized cellulose nanocrystal alginate composites

The poor mechanical properties of alginate when exposed to aqueous solution have been a problem plaguing researchers within the biomedical field. In order to be able to improve the mechanical properties in a systematic manner functionalized cellulose nanocrystals (CNCs) were added to alginate and UV‐induced crosslinked following an azo‐initiated free radical polymerization. CNCs were functionalized with 4‐pentenoic acid (PA‐g‐CNCs) using a simple, environmentally friendly solvent‐free esterification. The dimensional and crystallinity properties of PA‐g‐CNCs remained unchanged following esterification. Thermogravimetric analysis, Fourier transform infrared spectroscopy, and ¹³C nuclear magnetic resonance indicated that 4‐pentenoic acid was present on the surface of CNCs through bulk analysis. These PA‐g‐CNCs were then used in the creation of composites with an azo‐initiator to induce UV‐dependent crosslinking for the improvement of the mechanical properties of alginate. It was shown that the properties of alginate can be enhanced with the addition of functionalized CNCs to nanocomposites in mechanical testing in wet and dry conditions. These results suggest that the addition of PA‐g‐CNCs and crosslinking by UV‐dependent free radical polymerization improves the performance of alginate when tested in dry conditions, but without any apparent dependence to azo‐initiated crosslinking when exposed to water in regards to mechanical properties. © 2017 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2018 , 135, 45857.     

Effect of processing method on cellulose nanocrystal/polyethylene-co-vinyl alcohol composites

Cellulose nanocrystals (CNCs) have emerged as fillers of interest to the polymer nanocomposite community due to their inherent properties and renewable precursors. However, challenges persist to incorporate CNCs into polymer matrices due to component incompatibility and/or thermal stability limitations of the nanoparticles. Therefore, the objective of this research is to examine the efficacy of different processing methods in producing CNC/polymer composites. In this work, CNCs were incorporated into polyethylene-co-vinyl alcohol (EVOH) using either a solution casting method or a multi-step method involving the same solution casting method followed by a melt mixing step. The resulting neat EVOH and composite materials were characterized to understand how the viscoelastic character and mechanical properties were influenced by CNC loading and processing method. The results of characterization experiments and micromechanical modeling suggested that the nanoparticle networks produced by each method were different and that a combined solution-melt processing method is beneficial in producing composites with improved properties, particularly at higher CNC loadings. This processing strategy may be more broadly applied to other nanocomposites.