Cellulose Nanocrystals Content Research Articles

Phase Diagram of Pickering Emulsions Stabilized by Cellulose Nanocrystals.

Cellulose is a promising renewable and biocompatible biopolymer for stabilizing Pickering emulsions (PEs). In the present study, PEs were produced by low-frequency ultrasounds with cellulose nanocrystals (CNCs) and caprylic/capric triglycerides. Phase diagrams allowed to understand mechanisms of formation and long-term stabilization of PEs. Emulsion type, continuous phase viscosity, and yield of oil incorporation were studied after PEs formation. Droplet size, oil release, and stability were measured weekly up to 56 days of storage. Results showed that oil mass fraction above 70% w/w led to unstable W/O PEs. Lower oil mass fraction formed O/W PEs of stability depending on CNC content and oil mass fraction. Droplet size stability increased with CNCs/oil ratio. A very low CNCs/oil ratio led to phase separation and oil release. High CNC content stabilized oil droplets surface, increased aqueous phase viscosity, and prevented creaming. Highly stable PEs were produced for CNC content above 3% (w/w) and oil mass fraction below 50% (w/w). Mechanisms for PEs formation and stabilization were proposed for various CNC contents and oil mass fractions.

Production of cellulose nanocrystals from tomato pomace as a food waste and their application for stabilizing of Pickering emulsions

This study aimed to purify cellulose from tomato pomace and investigate properties of obtained cellulose nanocrystals (CNC) and their application for stabilization of Pickering emulsion. The tomato pomace was treated under alkaline and bleaching to produce purified cellulose and cellulose nanocrystals were then extracted by acid hydrolysis at different temperatures and times. The best CNC were obtained under acid hydrolysis at 45 °C and 30 min with crystallinity of 79%. Analysis of FTIR, TGA, and DSC was used to investigate the chemical and thermal properties of cellulose nanocrystals. TEM images showed spherical particles with average diameter of 104 ± 10 nm. To test the emulsifying ability of CNC, different concentrations of nanocrystals were applied to stabilize an oil in water Pickering emulsion. By increased the CNCs concentration, stability of the emulsions to physical stress, heat, and storage time increased. The results of this study showed that cellulose nanocrystals as an environmentally friendly material can be extracted from a food waste and have the ability to stabilize oil in water emulsions.

Enhancing mechanical and thermal properties of plasticized poly-L-(lactic acid) by incorporating aminated-cellulose nanocrystals

Cellulose nanocrystals (CNCs) have attracted much interest as a nucleating and reinforcing agent for poly-L-(lactid acid) (PLLA). However, the processing route to incorporate CNCs into PLLA matrices and the CNC content have a strong impact on the nucleating and reinforcing efficiency of the cellulose nanofillers (CNs). In the present work, a single melt-processing mode using poly(ethylene glycol) (PEG) as carrier for the CNCs and aminated CNCs (Am-CNCs), prepared via periodate oxidation followed by the addition of diaminododecane, was adopted to elaborate plasticized PLLA composites with different CN contents. The nucleating efficiency was investigated by differential scanning calorimetry using Avrami's approach to determine the half-crystallization time (t1/2). The influence of the CNC content on the mechanical properties and melt rheology was also assessed by tensile test and frequency sweep measurements. The incorporation of CNCs and Am-CNCs resulted in a marked enhancement in both tensile modulus and strength, with an optimal effect at 2% nanofiller content, and the best performance was observed for the Am-CNCs. A similar tendency was also observed for the melt rheology of the PLLA/PEG blend, which demonstrated a significant increase in both G′ and G′′ with respect to the neat PLLA/PEG matrix. The results were justified by the effective nucleating ability of the CNCs and their dispersion degree within the plasticized PLLA matrix.

Effect of different types of nanocellulose on the structure and properties of gelatin films

The use of nanocellulose to enhance the performance of biopolymer films is a recent trend in food packaging. This current study aims to investigate the impact of incorporating different morphologies of nanocellulose, namely cellulose nanofibrils (CNFs), cellulose nanospheres (CNSs), and cellulose nanocrystals (CNCs), on the structures and properties of gelatin film. The FTIR confirmed the formation of triple helix structures among CNF and CNC groups due to more hydrogen bonds generated between cellulose and gelatin molecules compared to CNSs. SEM analysis revealed a uniform distribution of CNCs in gelatin but aggregated with an increase in CNC contents, while CNF and CNS groups exhibited aggregation of cellulose upon the surface of gelatin because the vast surface area of nanospheres along with the nanofibrils structure led to irregular dispersion of cellulose (especially CNSs). In comparison to the CNF5% and CNS groups, CNC and CNF2% (w/w) groups greatly improved the mechanical characteristics of the gelatin films to 131.27% EAB and 20.71 MPa TS due to strong hydrogen bond interaction, more triple helix structures, and the relatively thorough dispersion of cellulose in the gelatin film. The incorporation of nanocellulose reduced the solubility and transparency of the gelatin films. Of all the films, CNC2% film exhibited a significant reduction of water vapor permeability due to the facile and even dispersion of CNCs in the gelatin network structure. Adding nanocellulose had little impact on the gelatin films’ heat stability. Therefore, the current work may be a new viable strategy for the construction of a novel molecular network system for enhancing the effectiveness of gelatin film containing lower content of CNCs.

Fabrication of well-dispersed cellulose nanocrystal reinforced biobased epoxy composites using reversibility of covalent adaptable network

Cellulose nanocrystal (CNC) shows great potential in reinforced composites but it is difficult to disperse in epoxy thermosets due to its poor dispersity in epoxy monomers. Herein, we reported a novel approach to disperse CNC in epoxidized soybean oil (ESO)-derived epoxy thermosets uniformly by using the reversibility of dynamic imine-containing ESO-derived covalent adaptable network (CAN). The crosslinked CAN was deconstructed by an exchange reaction with ethylenediamine (EDA) in dimethyl formamide (DMF), leading to a solution of deconstructed CAN with plenty of hydroxyl and amino groups, which could form strong hydrogen bonds with hydroxyl groups of CNC and thus facilitated and stabilized dispersion of CNC in the deconstructed CAN solution. Epoxy composite with well-dispersed CNC was finally achieved by a reformation of CAN through the removal of DMF and EDA. In this way, the epoxy composites with CNC content up to 30 wt% were successfully prepared and showed drastically reinforced mechanical properties. The tensile strength and Young's modulus of the CAN were improved by up to ∼70 % and ∼45 times with the incorporation of 20 and 30 wt% CNC, respectively. The composites showed excellent reprocessability without significant loss in mechanical properties after reprocessing.

Enhanced mechanical and thermal properties while maintaining transparency of epoxy resin film by introducing shear-oriented cellulose nanocrystals

Alignment of cellulose nanocrystals (CNCs) in the aqueous phase have been studied in depth. However, there are few reports on the orientation control of CNCs as rod-like nano fillers in epoxy resins. In this research, the rheological behavior of CNCs/epoxy resin system before curing indicating that CNCs in which can be oriented through shear-induced orientation. Based on this point, shear-oriented CNCs reinforced resin composite films were successfully prepared, mechanical properties, optical properties and thermal stability of which were systematically investigated. Firstly, mechanical properties of composite films can be significantly improved by introducing oriented CNCs at all CNC content. And the aspect ratio of oriented CNCs also has an obvious impact on their enhancement effect. Secondly, although their transmittance decreases with the increase of CNC content, it is possible to obtain composite films with a transmittance close to that of pure epoxy resin film by adjusting the preparation process of CNCs. Finally, the thermal stability of oriented CNCs reinforced epoxy resin composite films at low CNC content is improved, but then decreases with the increase of CNC content. The successful preparation of oriented CNCs reinforced epoxy resin composite films with better mechanical and thermal properties while maintaining transparency will be conducive to expanding the applications of epoxy resins reinforced with rod like micro/nano fillers.

Ice recrystallization inhibition effect of cellulose nanocrystals at constant and cycling temperatures

Understanding the effects of ice recrystallization inhibitors at varying temperatures is critical for evaluating their applications. We studied the ice recrystallization inhibition (IRI) effects of cellulose nanocrystals (CNCs) at constant and cycling temperatures. A splat assay using a 3.0 % sucrose solution showed that the IRI effect of 0.2 % CNCs decreased with increasing temperatures from −10 °C to −2 °C; the IRI effects of 0.5 % and 1.0 % CNCs remained unchanged for an increase in temperature from −10 °C to −4 °C but decreased at the temperature of −2 °C. A sandwich assay using a 25.0 % sucrose solution revealed that IRI effects increased with increasing temperatures, except in the presence of 0.2 % and 0.5 % CNCs at −5 °C and − 4 °C. A sandwich assay using a 35.0 % sucrose solution revealed that better IRI effects were observed at higher temperatures at all CNCs concentrations. At cycling temperatures, CNCs were inactive for storage times for ≤2 h, regardless of the rate, holding time, and amplitude of temperature fluctuation, but were active for storage times of 2 and 10 days. The IRI effects of CNCs at different temperatures may be related to the coverage of CNCs on ice surface, diffusion rate of CNCs to ice surface, and types of ice recrystallization.

Isotropic Gels of Cellulose Nanocrystals Grafted with Dialkyl Groups: Influence of Surface Group Topology from Nonlinear Oscillatory Shear

Attractive (non-self-assembling) aqueous cellulose nanocrystal (CNC) suspensions were topologically tailored into isotropic gels through the surface grafting of dialkyl groups. We thus focus on the influence of CNC concentration, including for pristine CNC, surface linker branching, branching degree, and the influence of side group size and branch-on-branch surface-grafted groups. The resulting mobility and strength of interaction in particle-particle interaction mediated by the surface groups was investigated from a rheological point of view. The emphasis is on nonlinear material parameters from Fourier-transform rheology and stress decomposition analysis. The results show that nonlinear material parameters are more sensitive than linear viscoelastic parameters to the onset of weakly interconnected networks in pristine CNC isotropic suspensions. All surface-modified CNC suspensions resulted in isotropic gels. The nonlinear material parameters were found to be broadly sensitive to CNC concentration, branching, degree of branching and surface-grafted linkers' length. However, the length of the grafted chains and the degree of branching were the primary factors influencing the nonlinear material response. Furthermore, the results showed evidence of two strain amplitude ranges with distinct nonlinear signatures that could be attributed to the disruption of weak network connection points and to distortions of more dense (aggregate) network regions, respectively.

Chitosan particles modulate the properties of cellulose nanocrystals through interparticle interactions: Effect of concentration

The physical and chemical properties of cellulose nanocrystals (CNC) were regulated by physical crosslinking with chitosan particles (CSp). At a fixed concentration (0.5 wt%) of CNC, varying CSp concentration (0.02–0.5 wt%) influenced the morphologies and chemical properties of the obtained complex particles (CNC-CSp). The results of Fourier transform infrared spectroscopy (FTIR) and zeta potential confirmed the electrostatic and hydrogen bonding interactions between CSp and CNC. At a low CSp concentration (0.02–0.05 wt%), the charge shielding effect induced the formation of particle aggregation networks, thus showing increased viscosity, turbidity and size (153.4–2605.7 nm). At a higher CSp concentration (0.1–0.5 wt%), the hydrogen bonding interaction promoted CSp adsorption onto the surface of CNC, thus facilitating the dispersion of CNC-CSp due to electrostatic repulsion caused by surface-adsorbed CSp. In addition, CSp improved the thermal stability, hydrophobicity (41.87–60.02°) and rheological properties of CNC. Compared with CNC, CNC-CSp displayed a better emulsifying ability and emulsion stability, in which CSp could play a dual role (i.e., charge regulator and stabilizer). This study suggests that introducing CSp can improve the properties and application potentials of CNC as food colloids.

Life cycle assessment and mechanical properties of nanocomposites based on cellulose nanocrystals

AbstractThe present work focuses on the preparation of cellulose nanocrystals (CNCs) reinforced composites based on polyhydroxybutyrate (PHB) and polypropylene (PP). The effects of the CNCs content as reinforcement and the addition of maleic anhydride (MA) as a coupling agent on the mechanical and morphological properties of the composites were studied. In addition, the biodegradability of the composites was investigated. Samples were prepared using PP and PHB as matrixes and CNCs as reinforcement. Test samples were prepared using the injection molding machine. The studied parameters were microscopic analysis and tensile strength measurement. Tensile strength increased with increasing CNC, but it decreased slightly when 5 wt% of CNC was added. Tensile strength decreased with the addition of MA. Environmental impacts from the production of 100 g of PP and PHB were evaluated using the life cycle assessment (LCA) approach. The results showed that the environmental impacts of composites containing PHB biopolymer are higher than PP ones.

Water-in-water Pickering emulsion stabilized by cellulose nanocrystals as space-confined encapsulating systems: From establishment to stability

The development of new water-in-water (W/W) emulsion systems and the improvement of the long-term stability of emulsions could create opportunities for studying interfacial bionic systems and microencapsulation applications. In this study, the new W/W emulsion systems were constructed from hydroxypropyl methylcellulose (HPMC) and maltodextrin (MD). The effects of cellulose nanocrystals (CNC) and environmental factors (ionic strength and pH) on the stability of W/W Pickering emulsions were investigated. The stabilizing effect was observed at contents of CNC as low as 0.025 wt%. The W/W Pickering emulsion showed no phase separation within 30 days when the CNC concentration was above 0.025 wt%, indicating that the emulsions were stable during the observation period. The stability of W/W Pickering emulsions was driven by the electrostatic repulsion provided by the CNC adsorbed at the droplet interface, which decreased with increasing NaCl concentration. This was attributed to the charge-shielding effect of NaCl weakening the electrostatic repulsion of the CNCs at the emulsion droplet interface. Lactobacillus helveticus cells were encapsulated in the W/W Pickering emulsion. These results revealed that the developed W/W Pickering emulsions have potential applications in protecting the activity of probiotic bacteria and investigating the behavior of cells in restricted spaces.

Fabrication of cellulose nanocrystal (CNC) from waste paper for developing antifouling and high-performance polyvinylidene fluoride (PVDF) membrane for water purification

Waste papers are used as a source of raw material to fabricate cellulose nanocrystals (CNCs), a highly valued product with a high degree of crystallinity. Rod-shaped CNCs with an average diameter of 53 ± 9 nm and an average length of 234 ± 42 nm were obtained with a crystallinity of around 78%. Polyvinylidene fluoride (PVDF) thin composite membrane was developed by adding CNCs into the PVDF matrix in different amounts (0, 0.5, 1, 1.5, 2, 3 wt%). Porous finger-like structures in the membrane increased with an increase in CNC content. The FTIR measurement and high-resolution FESEM image of the membranes verified the presence of CNCs in the composite membranes. 48% high pure water flux (PWF) was obtained for PVDF/CNC as compared to pristine PVDF membrane with the addition of 3% CNCs at a pressure of 1 kg−1cm−2. Water contact angle (WCA) also decreased from 85° to 69° with increasing the wt% of CNCs in the dope solution, which signifies improved hydrophilicity. Further, the PVDF/CNCs membrane showed a high bovine serum albumin (BSA) rejection of 93% and a flux recovery ratio (FRR) of 76.76 %, whereas the pristine PVDF membrane showed BSA rejection of 70.86% and a FRR of 40.82 %, respectively.

Development of chitosan/rice protein hydrolysates/ZnO nanoparticles films reinforced with cellulose nanocrystals

In the present work, the composite films were obtained by the solution casting method from chitosan and rice protein hydrolysates, reinforced with cellulose nanocrystals (CNC) of different contents (0 %, 3 %, 6 % and 9 %). The influence of different CNC loadings on the mechanical, barrier and thermal properties was discussed. SEM showed the formation of intramolecular interactions between the CNC and film matrices, leading to more compact and homogeneous films. These interactions had a positive influence on the mechanical strength properties, which was reflected in higher breaking force of 4.27 MPa. The elongation dwindled from 132.42 % to 79.37 % with increasing CNC levels. The linkages formed between the CNC and film matrices reduced the water affinity, leading to a reduction in their moisture content, water solubility and water vapor transmission. Thermal stability of the composite films was also improved in the presence of CNC, by increasing maximum degradation temperature from 311.21 to 325.67 °C with increasing CNC contents. The strongest DPPH inhibition of the film was 45.42 %. The composite films exhibited the highest inhibition zone diameter against E. coli (12.05 mm) and S. aureus (12.48 mm), and the hybrid of CNC and ZnO nanoparticles exhibited stronger antibacterial activity than their single existent forms. The present work shows the possibility of obtaining CNC-reinforced films with improved mechanical, thermal and barrier properties.

Self-healing waterborne polyurethane coatings with high transparence and haze via cellulose nanocrystal stabilized linseed oil Pickering emulsion

Protection coatings with self-healing ability can significantly enhance their anti-corrosion properties and service life. In this study, self-healing waterborne polyurethane (WPU) coatings with high transparence and haze were facile fabricated via cellulose nanocrystal (CNC) stabilized linseed oil (LO) Pickering emulsion. Sustainable CNCs displayed outstanding emulsifying ability and stability to stabilize LO Pickering emulsion. The size of LO Pickering emulsion droplets decreases with the CNC concentration, while the emulsion fraction and surface coverage by CNCs increase with CNC concentration, leading to a more stable Pickering emulsion. The self-healing rates of WPU coatings at varied time, temperature, CNC and catalyst concentration were investigated. Higher temperature, larger emulsion droplets, and with driers employed as catalysts generally lead to faster self-healing rate. The WPU self-healing coatings displayed much better abrasion resistance and mechanical properties than pristine WPU due to the incorporation of CNCs. Moreover, the WPU self-healing coatings show a high transparence and haze due to light scattering, and their applications as coatings of lamp covers and glass to achieve uniform light distribution and privacy protection with high light transmission were further demonstrated.

Formulation and stabilization of high internal phase emulsions: Stabilization by cellulose nanocrystals and gelatinized soluble starch

In this work, high internal phase emulsions (HIPEs) stabilized by naturally derived cellulose nanocrystals (CNC) and gelatinized soluble starch (GSS) were fabricated to stabilize oregano essential oil (OEO) in the absence of surfactant. The physical properties, microstructures, rheological properties, and storage stability of HIPEs were investigated by adjusting CNC contents (0.2, 0.3, 0.4 and 0.5 wt%) and starch concentration (4.5 wt%). The results revealed that CNC–GSS stabilized HIPEs exhibited good storage stability within one month and the smallest droplets size at a CNC concentration of 0.4 wt%. The emulsion volume fractions of 0.2, 0.3, 0.4 and 0.5 wt% CNC–GSS stabilized HIPEs after centrifugation reached 77.58, 82.05, 94.22, and 91.41 %, respectively. The effect of native CNC and GSS were analyzed to understand the stability mechanisms of HIPEs. The results revealed that CNC could be used as an effective stabilizer and emulsifier to fabricate the stable and gel-like HIPEs with tunable microstructure and rheological properties.

Depletion interaction may reduce ice recrystallization inhibition activity of cellulose nanocrystals (CNCs) at high concentrations

In ice cream, food hydrocolloids are commonly used as stabilizers for controlling ice recrystallization. Recent studies suggest that some stabilizers might bind to ice crystal surfaces and inhibit recrystallization. However, this ice-binding mechanism is challenged by the fact that stabilizers at high concentrations sometimes have reduced activity or even accelerate ice recrystallization. In this work, we determined the ice recrystallization inhibition (IRI) activity of cellulose nanocrystals (CNCs) at different concentrations in the 3.0% sucrose solution by the splat assay and in the 25.0% and 40.0% sucrose solutions by the sandwich assay. Reduced activity at high CNCs concentrations was observed in the sandwich assay. It was not linked to the phase separation or liquid crystal phase formation of CNCs but was caused by the accretion of nearby ice crystals and the forming of large ice crystals with irregular morphology and high aspect ratios. A new explanation based on the depletion-interaction-induced accretion of ice crystals was proposed. Our findings might resolve the contradiction between the ice-binding mechanism and the stabilizer concentration effect and add more support to the interfacial mechanism of ice recrystallization inhibition. They also pointed out the importance of selecting suitable stabilizer concentrations for screening IRI active materials and manufacturing frozen desserts.

The Fabrication of Gelatin-Elastin-Nanocellulose Composite Bioscaffold as a Potential Acellular Skin Substitute.

Gelatin usage in scaffold fabrication is limited due to its lack of enzymatic and thermal resistance, as well as its mechanical weakness. Hence, gelatin requires crosslinking and reinforcement with other materials. This study aimed to fabricate and characterise composite scaffolds composed of gelatin, elastin, and cellulose nanocrystals (CNC) and crosslinked with genipin. The scaffolds were fabricated using the freeze-drying method. The composite scaffolds were composed of different concentrations of CNC, whereas scaffolds made of pure gelatin and a gelatin-elastin mixture served as controls. The physicochemical and mechanical properties of the scaffolds, and their cellular biocompatibility with human dermal fibroblasts (HDF), were evaluated. The composite scaffolds demonstrated higher porosity and swelling capacity and improved enzymatic resistance compared to the controls. Although the group with 0.5% (w/v) CNC recorded the highest pore size homogeneity, the diameters of most of the pores in the composite scaffolds ranged from 100 to 200 μm, which is sufficient for cell migration. Tensile strength analysis revealed that increasing the CNC concentration reduced the scaffolds' stiffness. Chemical analyses revealed that despite chemical and structural alterations, both elastin and CNC were integrated into the gelatin scaffold. HDF cultured on the scaffolds expressed collagen type I and α-SMA proteins, indicating the scaffolds' biocompatibility with HDF. Overall, the addition of elastin and CNC improved the properties of gelatin-based scaffolds. The composite scaffolds are promising candidates for an acellular skin substitute.

Green remediation of cadmium-contaminated soil by cellulose nanocrystals.

Cellulose nanocrystals (CNC) were used as a novel, green eluent to remediate Cd-contaminated soil in this study. The influence of washing conditions on the removal of Cd, including CNC concentration, pH value, liquid/solid (L/S) ratio, contact time and temperature were investigated. The effect of CNC remediation of Cd-contaminated soil on soil health and the possible remediation mechanism were also explored. The results showed that CNC concentration, pH value and contact time had a significant effect on the removal efficiency of Cd. CNC rapidly removed heavy metals in soil within 30min. When the pH value of the eluent was 9.0, the removal efficiency of Cd could reach 86.3%. The eluent mainly removed exchangeable and reducible fractions of Cd, which could effectively reduce the bioavailability of heavy metals. CNC washing had no negative effects on seed growth, species abundance and Shannon index. C-O, -COO- groups on CNC played an important role in the reaction between CNC and soil Cd, and other oxygen-containing functional groups on CNC could also assist in adsorption, ion exchange and chemical complexation processes. Therefore, cellulose nanocrystals had the potential to remediate heavy metal-contaminated soils in a green and efficient manner.

Influences of modified fiber inclusion with varying particle size on corn starch-based extrudate expansion.

The inclusion of cellulose nanocrystals (CNC) and microcrystalline cellulose (MCC) during extrusion processing of corn starch (CS) is presented in this study. Blends were prepared by incorporating CNC and MCC at different concentrations, 1%, 3%, 5%, and 10% w/w in CS. The crystallinity index (CrI) of CNC and MCC was determined using X-ray diffraction, and the chemical functionality of CNC, MCC, and CS was studied using Fourier transform infrared spectroscopy. The pasting properties of the blends were studied using Micro Visco-Amylo-Graph before extrusion. The blends were preconditioned to 18±0.5% (w.b.) moisture and extruded using a twin-screw extruder at 200 and 250rpm at 140°C. CS-CNC's expansion ratio (ER) values were 2.95 to 3.35 and 2.72 to 3.22 for MCC. CNC's CrI and particle size were significantly lower than MCC, allowing CNC-based extrudates to have ER values similar to the control even at high CNC concentration (≤10% w/w). This study demonstrated that fiber with particle size<100µm can be added in direct-expanded product formulations at high concentrations without negatively influencing the extrudate texture while offering increased nutritional value. PRACTICAL APPLICATION: This study gives insight into the potential application of cellulose nanocrystals and microcrystalline cellulose in manufacturing direct-expanded extruded products, providing high fiber content without compromising the product quality. This knowledge could also be translated into manufacturing other food products such as breakfast cereals, pasta, and bread.

Crystallization and mechanical property of fully biobased poly(hexamethylene 2,5-furandicarboxylate)/cellulose nanocrystals composites

Through a common solution and casting method, novel fully biobased poly(hexamethylene 2,5-furandicarboxylate) (PHF)/cellulose nanocrystals (CNC) composites were prepared in this research at low contents of CNC. Scanning electron microscopy result showed that CNC uniformly dispersed in the PHF matrix without obvious aggregations, even CNC content reached 1 wt%. CNC, as a relatively effective heterogeneous nucleating agent, promoted the melt crystallization of PHF under different conditions. In addition, to explore the nucleation effect, the nucleation activity as well as the nucleation efficiency of CNC were quantitively determined. In the composites, the crystallization mechanism and crystal structure of PHF remained unchanged despite the presence of CNC. Low loadings of CNC improved both the Young's modulus and the yield strength of PHF to some degree, indicating that CNC nanofiller reinforced PHF matrix. In sum, CNC improved both the crystallization and the mechanical property of PHF, favoring the potential wider application of PHF/CNC composites due to the fully biobased feature.