Chemically modified cellulose micro- and nanofibrils as paper-strength additives

Chemically modified cellulose micro- and nanofibrils were successfully used as paper strength additives. Three different kinds of cellulose nanofibrils (CNFs) were studied: carboxymethylated CNFs, periodate-oxidised carboxymethylated CNFs and dopamine-grafted carboxymethylated CNFs, all prepared from bleached chemical fibres of dissolving grade, and one microfibrillated cellulose from unbleached kraft fibres. In addition to mechanical characterization of the final paper sheets the fibril retention, sheet density and sheet morphology were also studied as a function of addition of the four different cellulose fibrils. In general, the cellulose fibrils, when used as additives, significantly increased the tensile strength, Young’s modulus and strain-at-break of the paper sheets. The effects of the different fibrils on these properties were compared and evaluated and used to analyse the underlying mechanisms behind the strengthening effect. The strength-enhancing effect was most pronounced for the periodate-oxidised CNFs when they were added together with polyvinyl amine (PVAm) or poly(dimethyldiallylammonium chloride) (pDADMAC). The addition of periodate-oxidised CNFs, with pDADMAC as retention aid, resulted in a 37% increase in tensile strength at a 2 wt% addition and an 89% increase at a 15 wt% addition (from 67 to 92 and 125 kNm/kg, respectively) compared to a reference with only pDADMAC. Wet-strong sheets with a wet tensile index of 30 kNm/kg were also obtained when periodate-oxidised CNFs and PVAm were combined. This significant increase in wet strength is suggested to be the result of a formation of cross-links between the aldehyde groups, introduced by the periodate oxidation, and hydroxyl groups on the lignocellulosic fibres and the primary amines of PVAm. Even though less significant, there was also an increase in wet tensile strength when pDADMAC was used together with periodate-oxidised fibrils which shows that the aldehyde groups are able to increase the wet strength without the presence of the primary amines of the PVAm. As an alternative method to strengthen the fibre network, carboxymethylated CNFs grafted with dopamine, by an ethyl dimethylaminopropyl carbodiimide coupling, were used as a strength additive. When used as an additive, these CNFs showed a strong propensity to form films on and around the fibres and significantly increased the mechanical properties of the sheets. Their addition resulted in an increase in the Young´s modulus by 41%, from 5.1 to 7.2 GPa, and an increase in the tensile strength index of 98% (from 53 to 105 kNm/kg) with 5 wt% retained dopamine-grafted CNFs.     

Fabrication and characterization of carboxylated cellulose nanocrystals reinforced glutenin nanocomposite

The non-biodegradable and non-renewable nature of plastic packaging has led to increasing interest in packaging materials based on bio-nanocomposites (biopolymer matrix reinforced with nanofillers). One such material is wheat gluten and its components. In this study we investigated nanocomposite materials prepared by casting a mixture of extracted glutenin from wheat gluten as the matrix and different concentrations of 2,2,6,6-tetramethylpiperidine-1-oxy radical (TEMPO)-carboxylated cellulose nanocrystals (C-CNC) as the reinforcing agent. The resulting films were characterized for their thermomechanical and barrier properties. Scanning electron microscopy (SEM) observations confirmed that the filler was homogeneously distributed in the matrix at the low and medium loadings, but some agglomerates and voids were visible at concentrations > 5 wt%. The mechanical properties showed that the presence of C-CNC (5 wt%) resulted in an increase (58.8 %) in tensile strength (TS) of glutenin films while at higher contents, the TS tended to decrease because of partial agglomeration of the filler. These effects were also reflected in the dynamic mechanical analysis (DMA) results and at a 5 wt% loading of nanocrystals the glutenin film gave the highest storage modulus (E′). The results obtained from differential scanning calorimetry (DSC) curves indicated that increasing the amount of C-CNC from 0 to 10 wt% led to an increase in glass transition temperature (T_g) from ?29.8 to ?23.7 °C. Although the use of C-CNC reduced the resistance to water vapor permeability (WVP) and water absorbance (WA), its incorporation up to 5 wt% resulted in composites with the lowest weight loss in water (WL). These results demonstrated that nanocellulose can reinforce glutenin polymers and that this system has potential as a packaging material, although much further study is needed.     

Nanocrystalline cellulose acetate (NCCA)/graphene oxide (GO) nanocomposites with enhanced mechanical properties and barrier against water vapor

Highly flexible nanocomposite films of nanocrystalline cellulose acetate (NCCA) and graphene oxide (GO) were synthesized by combining NCCA and GO sheets in a well-controlled manner. By adjusting the GO content, various NCCA/GO nanocomposites with 0.3–1 wt% GO were obtained. Films of these nanocomposites were prepared using the solvent casting method. Microscopic and X-ray diffraction (XRD) measurements demonstrated that the GO nanosheets were uniformly dispersed in the NCCA matrix. Mechanical properties of the composite films were also studied. The best GO composition of the samples tested was 0.8 wt%, giving tensile strength of 157.49 MPa, which represents a 61.92 % enhancement compared with NCCA. On the other hand, the composite films showed improved barrier properties against water vapor. This simple process for preparation of NCCA/GO films is attractive for potential development of high-performance films for electrical and electrochemical applications.     

Nanofibrillated cellulose/nanographite composite films

Though research into nanofibrillated cellulose (NFC) has recently increased, few studies have considered co-utilising NFC and nanographite (NG) in composite films, and, it has, however been a challenge to use high-yield pulp fibres (mechanical pulps) to produce this nanofibrillar material. It is worth noting that there is a significant difference between chemical pulp fibres and high-yield pulp fibres, as the former is composed mainly of cellulose and has a yield of approximately 50 % while the latter is consist of cellulose, hemicellulose and lignin, and has a yield of approximately 90 %. NFC was produced by combining TEMPO (2,2,6,6-tetramethypiperidine-1-oxyl)-mediated oxidation with the mechanical shearing of chemi-thermomechanical pulp (CTMP) and sulphite pulp (SP); the NG was produced by mechanically exfoliating graphite. The different NaClO dosages in the TEMPO system differently oxidised the fibres, altering their fibrillation efficiency. NFC–NG films were produced by casting in a Petri dish. We examine the effect of NG on the sheet-resistance and mechanical properties of NFC films. Addition of 10 wt% NG to 90 wt% NFC of sample CC2 (5 mmol NaClO CTMP-NFC homogenised for 60 min) improved the sheet resistance, i.e. from that of an insulating pure NFC film to 180 Ω/sq. Further addition of 20 (CC3) and 25 wt% (CC4) of NG to 80 and 75 wt% respectively, lowered the sheet resistance to 17 and 9 Ω/sq, respectively. For the mechanical properties, we found that adding 10 wt% NG to 90 wt% NFC of sample HH2 (5 mmol NaClO SP-NFC homogenised for 60 min) improved the tensile index by 28 %, tensile stiffness index by 20 %, and peak load by 28 %. The film’s surface morphology was visualised using scanning electron microscopy, revealing the fibrillated structure of NFC and NG. This methodology yields NFC–NG films that are mechanically stable, bendable, and flexible.     

Transparent montmorillonite/cellulose nanofibril nanocomposite films: the influence of exfoliation degree and interfacial interaction

To obtain high performance of nanocomposite films made of cellulose nanofibrils (CNFs) and montmorillonites (MMTs), highly ordered nanostructures and abundant interfacial interactions are of extreme importance, especially for CNF film with high MMT content. Here, we tend to unveil the influence of exfoliation degree of MMTs and their interfacial interactions with CNFs on the properties of ensuing nanocomposite films. Monolayer MMTs (ML-MMTs) prefer to form highly ordered nanostructure during water evaporation induced self-assembly. The obtained nanocomposite film with 30 wt% ML-MMTs exhibits a tensile strength of 132 MPa, a total light transmittance of 90.2% (550 nm), and water vapor transmission rate (WVTR) of 41.5 g mm/m² day, better than the film made of original MMTs (O-MMTs) and CNFs (30 MPa strength, 60% transparency, and 78.7 g mm/m² day WVTR). Moreover, the physical properties (153 MPa strength and 20.9 g mm/m² day WVTR) of nanocomposite film can be further enhanced by constructing ionic interactions between the ML-MMT and CNF using 0.5 wt% cationic polyethylenimine (PEI). However, as the amount of PEI continues to increase, its performance will be deteriorated dramatically because of the disordered orientation of ML-MMTs. This work could provide an insight into the fabrication of high performance MMT/CNF nanocomposite film for advanced applications.

Graphical abstract

     

Length-controlled cellulose nanofibrils produced using enzyme pretreatment and grinding

The length of cellulose nanofibrils (CNFs) is a significant parameter for various applications. The goal of this research was to employ a fabrication method to produce length-controlled CNFs; the chosen technique was enzy-grinding (enzyme pretreatment followed by mechanical grinding). Here, we presented the results of the optimization of the diameter and length, the characterization of the properties of CNFs and nanofilms prepared using these fibrils. The cellulose morphology, crystallinity index (CrI), chemical structure, and thermal stability were investigated as functions of the enzyme loading and hydrolysis time. The results showed that enzy-grinding could effectively reduce the diameter and length of cellulose fibrils. The average diameter was about 8.6 ± 3.6 nm, and the length could be controlled over the range from 0.76 ± 0.38 μm to ≥ 4 μm (i.e. aspect ratios from 43 to ≥ 328). After the grinding process, the CNFs maintained high thermal stability and no change in the chemical structure compared to the original pulp. The transmittance and mechanical properties of the CNF films were strongly dependent on the fibril length. The fabrication of length-controlled CNFs using the enzy-grinding process is meaningful and significant research which could be relevant to the optimization of such materials for various applications.     

Antibacterial cellulose acetate films incorporated with N‐halamine‐modified nano‐crystalline cellulose particles

Cellulose acetate (CA) membranes have been widely used as food packaging materials as well as reverse osmosis systems. This study presents the manufacturing of composite CA film with antibacterial properties which is essential for CA film applications in the industry. N‐Halamine precursor of polymethacrylamide‐modified nano‐crystalline cellulose particles (NCC‐PMAMs) were prepared and incorporated into CA film. The composite films with intercalated structure were formed via a solvent‐casting technique. After chlorination, the composite film CA/NCC‐PMAM‐Cl‐1.0 with 1.82 × 10¹⁶ atoms/cm² covalently bonded chlorine showed excellent antibacterial properties by inactivating 6.04 logs of Staphylococcus aureus and 6.27 logs of Escherichia coli within 10 and 5 min, respectively. According to X‐ray diffraction spectra, NCC‐PMAMs behaved as a facilitator for film crystallization. The mechanical strength of the composite film also increased compared with that of pure CA film. However, the composite film became brittle and the maximum decomposition temperature decreased slightly. Preliminary data of in vitro cytocompatibility evaluation indicate that the film is not toxic and has potential use in food packaging. Copyright © 2016 John Wiley & Sons, Ltd.     

Water redispersible cellulose nanofibrils adsorbed with carboxymethyl cellulose

Cellulose nanofibrils (CNFs) are difficult to redisperse in water after they have been completely dried due to the irreversible agglomeration of cellulose during drying. Here, we have developed a simple process to prepare water-redispersible dried CNFs by the adsorption of small amounts of carboxymethyl cellulose (CMC) and oven drying. The adsorption of CMC onto CNFs in water suspensions at 22 and 121 °C was studied, and the adsorbed amount of CMC was measured via conductimetric titration. The water-redispersibility of dried CNFs adsorbed with different amounts of CMC was characterized by sedimentation test. Above a critical threshold of CMC adsorption, i.e. 2.3 wt%, the oven dried CNF–CMC sample was fully redispersible in water. The morphology, rheological, and mechanical properties of water-redispersed CNF–CMC samples were investigated by field emission scanning electron microscopy, viscosity measurement, and tensile test, respectively. The water-redispersed CNFs preserved the original properties of never dried CNFs. This new method will facilitate the production, transportation and storage, and large-scale industrial applications of CNFs.     

The transparency and mechanical properties of cellulose acetate nanocomposites using cellulose nanowhiskers as fillers

Cellulose nanowhiskers (CNWs) were chemically modified by acetylating to obtain acetylated cellulose nanowhiskers (ACNWs) which could be well dispersed in acetone. The chemical modification was limited only on the surface of CNWs which was confirmed by transmission electron microscopy (TEM) and X-ray diffraction (XRD). Surface substitution degree of ACNWs was evaluated to be 0.45 through X-ray photoelectron spectroscopy (XPS). Fully bioresource-based nanocomposite films were manufactured by incorporation of ACNWs into cellulose acetate (CA) using a casting/evaporation technique. Scanning electron microscope (SEM) demonstrated that ACNWs dispersed well in the CA matrix, which resulted in high transparency of all CA nanocomposites. The tensile strength, Young’s modulus and strain at break of all CA nanocomposites exhibited simultaneous increase in comparison with neat CA matrix. At the content of 4.5 wt% ACNWs, the tensile strength, Young’s modulus and strain at break of the CA nanocomposite film were increased by 9, 39, and 44 % respectively.     

Tensile,thermal, and antibacterial characterization of composites of cellulose/modified Pennisetum purpureum natural fibers with in situ generated copper nanoparticles

Eco-friendly all cellulose composites were developed using cellulose as matrix and nanocomposite (in situ generated copper nanoparticles modified Napier Grass Fibers (NGFs)) as fillers for the antibacterial applications. The content of the nanocomposite filler was increased from 1?wt.% to 5?wt.% in the cellulose matrix. All these composites were characterized by Scanning Electron Microscopy (SEM), Tensile, Thermo Gravimetric Analysis (TGA), and antibacterial tests. SEM-EDX analysis revealed the in situ generation of copper nanoparticles on the surface of the films. Further, all cellulose composites showed good thermal stability. A minimum of 30% increase in char residue was observed in all cellulose nanocomposites compared to matrix. Antibacterial analysis indicated an excellent clear zone formation against both Gram Negative (Escherichia coli) and Gram Positive (Staphylococcus) bacteria. Hence, all these cellulose nanocomposite films can be considered as antibacterial packaging and dressing materials in medical field.     

Eco-friendly synthesis, characterization and properties of a sodium carboxymethyl cellulose/graphene oxide nanocomposite film

A previously unreported nanocomposite (CMC/GO) high-performance film was prepared by a simple solution mixing-evaporation method. The structure, thermal stability, and mechanical properties of the composite films were investigated by wide-angle X-ray diffraction, Fourier transform infrared spectroscopy, Raman spectroscopy, scanning electron microscopy, thermogravimetry analysis, and mechanical testing. The results obtained from these different studies revealed that CMC and graphene oxide were able to form a homogeneous mixture. Compared with pure CMC, the tensile strength and Young’s modulus of the graphene-based materials were improved significantly upon incorporation of 1 wt% graphene oxide by 67 ± 6 % and 148 ± 5 %, respectively. In addition, the DMA composite films also showed a high storage modulus up to 250 °C.     

Dual-functional chitosan–methylisothiazolinone/microfibrillated cellulose biocomposites for enhancing antibacterial and mechanical properties of agar films

In order to enhance the antibacterial and mechanical properties of agar films, the chitosan-methylisothiazolinone (C–MIT) complex was first prepared by the ionic gelation method, and the characterization of the C–MIT complex was carried out by Fourier transform infrared spectroscopy, transmission electron microscopy, and Thermo gravimetry. Chitosan was successfully crosslinked with tripolyphosphate for the nanoencapsulation of methylisothiazolinone, and the C–MIT complex was spherical in shape with a diameter of about 10 nm. The C–MIT/MFC biocomposites obtained through the adsorption of the C–MIT complex on the microfibrillated cellulose (MFC) was then incorporated into the agar films. In comparison with the pure agar films, the tensile strength of the agar composite films was increased by about 19 % at the loading of 10 wt% of C–MIT/MFC biocomposites, and antibacterial tests demonstrated that the agar composite films exhibited remarkable antibacterial activities against both Escherichia coli and Staphylococcus aureus. This work provides a new approach to utilizing multifunctional agar films in the medical field.     

Mechanical,thermal and barrier properties of pectin/cellulose nanocrystal nanocomposite films and their effect on the storability of strawberries (Fragaria ananassa)

In this work, two formulations of pectin/cellulose nanocrystals/glycerol nanocomposites were employed as packaging to extend storage life of strawberries. The effects of incorporating cellulose nanocrystals extracted from bleached Kraft wood pulp on the mechanical, thermal, and barrier properties of pectin‐based nanocomposites were evaluated. Nanocomposite films with different filler levels of cellulose nanocrystals (1, 2, 4 and 8% w/w) were prepared by casting. Compared with the neat film of pectin, improvements in the mechanical properties of the nanocomposites were observed, but these films became fragile. To improve the film flexibility, glycerol was added as a plasticizer and then new variations in the mechanical, thermal, and barrier properties of these nanocomposites were evaluated. The effects of nanocomposite films on storability of strawberries were compared with Poly vinyl chloride packaging films. The Poly vinyl chloride film and the nanocomposites showed similar behavior regarding weight loss by the strawberries, especially in the initial days of storage. The results show that pectin/cellulose nanocrystals/glycerol nanocomposites could be considered as a viable packaging alternative for replaced the Poly vinyl cloride film. Copyright © 2015 John Wiley & Sons, Ltd.     

Highly flexible, transparent cellulose composite films used in UV imprint lithography

Highly flexible, optically transparent epoxy resin/cellulose composites were prepared by using the solution impregnation method firstly and then thermal cured. The composite contained 60 wt% resin was still mechanically stable and flexible, and it integrated the merits of cellulose and resin, but the highly hydrophilic behavior of cellulose has been reduced. Contact angle measurements with water demonstrated that the composite films had obvious hydrophobic properties, and a decrease in the water uptake and the permeability towards water vapor gas was also observed. The transmittance of the composite films at 550 nm was about 85–88 %. The thermal and mechanical properties of the composite films were improved. Moreover, the composite films could be used in UV imprint lithography for circuit, and the definition could be compared with that of widely used glass plate.     

Synergistic effect of graphene oxide nanoplatelets and cellulose nanofibers on mechanical,thermal, and barrier properties of thermoplastic starch

In recent years, because of the limited availability of oil resources and the increasing concerns regarding environment protection, much attention has been drawn to produce packaging films based on degradable biopolymers instead of synthetic polymers. On the other hand, because of the high costs of oil extraction, raw materials and film production, and disposing of the waste products of synthetic films, the need to replace these films with less pollutant and more cost‐effective films is growing globally. In this study, to answer the need for replacing synthetic polymer films, nanocomposite films based on thermoplastic starch reinforced with cellulose nanofibers and graphene oxide nanoplatelets were produced and characterized. The results implied that the synergistic effect of cellulose nanofibers and graphene oxide nanoplatelets has played an important role in improving the mechanical properties of the films. The results showed that with the addition of cellulose nanofibers and graphene oxide nanoplatelets, the tensile strength and elastic modulus of starch film were increased from 3 and 32 MPa to 13 and 436 MPa, which corresponds to 438% and 1435% improvement, respectively. In addition, the oxygen permeability resistance and the water vapor transmission for samples containing 3 wt% of graphene oxide nanoplatelets was decreased by 78% and 30% compared with the thermoplastic starch film, respectively. The permeability coefficient of the samples containing 3 wt% graphene oxide nanoplatelets for oxygen, nitrogen, and carbon dioxide have proved to be 0.051, 0.054, and 0.047 barrer, which shows that these films can perform well as packaging films.     

Properties of poly(acrylamide)/TEMPO-oxidized cellulose nanofibril composite films

Self-standing composite films consisting of 2,2,6,6-tetramethylpiperidine-1-oxyl-oxidized cellulose nanofibril (TOCN) and anionic poly(acrylamide) (PAM) in various weight ratios were prepared by casting and drying of homogeneous mixtures of aqueous TOCN dispersion and PAM solution. PAM/TOCN composite films consisting of 25 % PAM and 75 % TOCN had clearly higher Young’s modulus (13.9 GPa) and tensile strength (266 MPa) than 100 % TOCN film (10.8 GPa and 223 MPa, respectively) or 100 % PAM film (4.9 GPa and 78 MPa, respectively), showing that PAM molecules have mechanical reinforcement ability in TOCN matrix. Some attractive interactions are likely formed between TOCN element surfaces and PAM molecules. In contrast, no such mechanical improvements were observed for poly(vinyl alcohol)/TOCN or oxidized starch/TOCN composite films prepared as references. Moreover, the mechanical properties of the PAM/TOCN composite films were further improved by controlling molecular mass and branching degree of the PAM. The high optical transparency and low coefficient of thermal expansion of the 100 % TOCN film were mostly maintained in the TOCN composite film containing 25 % PAM.     

Facile synthesis of microfibrillated cellulose/organosilicon/polydopamine composite sponges with flame retardant properties

Cellulose composite sponges with good mechanical, heat-insulating and flame retardant properties were constructed by a facile method. Simultaneous polymerization of dopamine and hydrolysis of organosilicon in the suspension of microfibrillated cellulose could provide the stiffness and flame ratardancy of the composite sponges. The hybrid sponges had low density (15.1–28.5 mg/cm³) and desirable compression strength (76.6–135.8 kPa). Scanning electron microscopy (SEM) and thermal conductivity tests revealed that the sponges are composed of a three-dimensional cellulosic network and the porous structure endowed them low thermal conductivity [~0.046 W/(m K)]. With the addition of organosilicon (45 wt%) and polydopamine (PDA) (10 wt%), a 456% improvement in BET surface area of the sponge could be achieved. The limiting oxygen index (LOI) of the composite sponge could be as high as 29.5 with 15 wt% PDA and could self-extinguish at once when it was removed from torch. That was owing to the promoted materials carbonization ability of silicon and radical scavenging activity of dopamine.     

Efficient alternative of antimicrobial nanocomposites based on cellulose acetate/Cu-NPs

The current research presents an efficient, cheap, and safe antimicrobial material for widespread use based on copper nanoparticles (Cu-NPs) loaded on cellulose acetate (CA) matrix. A reduction process of CuSO₄·5H₂O has been performed to prepare Cu-NPs. The nanosized copper particles included oxidized Cu (15–20 nm). Two different loads of Cu-NPs were used in this study, 2% and 6% mol.%. The presence of Cu-NPs incorporated with CA films slightly affected the tensile index of the films, where low and high-loaded Cu-NPs enhanced the tensile index by small values ranged from 0.640 to 0.650 and 0.667, respectively. A study on the antibacterial activity of these nanocomposites was carried out for Staphylococcus aureus, Pseudomonas aeruginosa, and Candida albicans. It has been found that CA containing Cu-NPs (2%) exhibited the highest antimicrobial activity against all test microbes including S. aeureus (21 mm), P. aeruginosa (18 mm), C. albicans (19 mm), and Aspergillus niger (15 mm). Results also revealed that CA film with 6% exhibited lower activity than film with 2% Cu-NPs. The morphological properties of CA/Cu-NPs films were characterized by scanning electron microscopy and transmission electron microscope in addition to X-ray diffraction. Low-loaded Cu-NPs showed homogenous distribution through CA matrix while, the high-loaded Cu-NPs were agglomerated through CA matrix. Thermal properties illustrated the enhancement of thermal stability of the film with increasing the loaded Cu-NPs.     

Anomalous reinforcing effects in cellulose gel-based polymeric nanocomposites

Cellulose-synthetic polymer nanocomposite films were prepared by immersion of cellulose gel in polymer solutions followed by dry casting. The cellulose hydrogel was prepared from aqueous alkali-urea solution. As the synthetic polymer, polystyrene (PS) and poly(methyl methacrylate) (PMMA) were used. The polymer content could be changed between 10 and 80% by changing polymer concentration of immersing solution. While the mechanical properties of the cellulose-PMMA composite films showed a nearly linear dependence on PMMA content, those of cellulose-PS composites showed an anomalous behavior; both tensile strength and Young’s modulus showed prominent maxima at 15–30 wt% PS contents. This anomaly may have resulted from the specific interaction between the aromatic ring of PS and the hydrophobic plane of the glucopyranoside. Both PMMA and PS composite films showed significant improvements in dimensional thermal stability; up to 25 wt% synthetic polymer content, the coefficient of thermal expansion (CTE) was as low as ca. 30 ppm/K, about 1/3 of the pure polymers. This indicates that the regenerated cellulose network is effective in suppressing thermal expansion of the synthetic polymers.     

Influence of high loading of cellulose nanocrystals in polyacrylonitrile composite films

Polyacrylonitrile-co-methacrylic acid (PAN-co-MAA) and cellulose nanocrystal (CNC) composite films were produced with up to 40 wt% CNC loading through the solution casting method. The rheological properties of the solution/suspensions and the structural, optical, thermal, and mechanical properties of the resulting films were investigated. The viscosity of the composite suspensions increased with higher CNC loadings and with longer aging times. PAN-co-MAA/CNC films maintained a similar level of optical transparency even with up to 40 wt% CNC loading. The glass transition temperature (Tg) increased from 92 to 118 °C, and the composites had higher thermal stability below 350 °C compared to both neat PAN-co-MAA and neat CNC. The mechanical properties also increased with higher CNC loadings, elastic modulus increased from 2.2 to 3.7 GPa, tensile strength increased from 75 to 132 MPa, and the storage modulus increased from 3.9 to 10.5 GPa. Using the Kelly and Tyson model the interfacial shear strength between the PAN-co-MAA and CNC was calculated to be 27 MPa.