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The cost-effective implementation of nanofibrillated cellulose (CNF) at industrial scale requires optimizing the quality of the nanofibers according to their final application. Therefore, a portfolio of CNFs with different qualities is necessary, as well as further knowledge about how to obtain each of the main qualities. This paper presents the influence of various production techniques on the morphological characteristics and properties of CNFs produced from a mixture of recycled fibers. Five different pretreatments have been investigated: a mechanical pretreatment (PFI refining), two enzymatic hydrolysis strategies, and TEMPO-mediated oxidation under two different NaClO concentrations. For each pretreatment, five high-pressure homogenization (HPH) conditions have been considered. Our results show that the pretreatment determines the yield and the potential of HPH to enhance fibrillation and, therefore, the final CNF properties. These results enable one to select the most effective production method with the highest yield of produced CNFs from recovered paper for the desired CNF quality in diverse applications.

This study aims to provide a comprehensive understanding of the key factors influencing the rheological behavior and the mechanisms of natural polyelectrolyte complexes (PECs) as flocculation agents for cellulose microfibers (CMFs) and nanofibers (CNFs). PECs were formed by combining two polyelectrolytes: xylan (Xyl) and chitosan (Ch), at different Xyl/Ch mass ratios: 60/40, 70/30, and 80/20. First, Xyl, Ch, and PEC solutions were characterized by measuring viscosity, critical concentration (c*), rheological parameter, ζ-potential, and hydrodynamic size. Then, the flocculation mechanisms of CMF and CNF suspensions with PECs under dynamic conditions were studied by measuring viscosity, while the flocculation under static conditions was examined through gel point measurements, floc average size determination, and ζ-potential analysis. The findings reveal that PEC solutions formed with a lower xylan mass ratio showed higher intrinsic viscosity, higher hydrodynamic size, higher z-potential, and a lower c*. This is due to the high molecular weight, charge, and gel-forming ability. All the analyzed solutions behave as a typical non-Newtonian shear-thinning fluid. The flocculation mechanisms under dynamic conditions showed that a very low dosage of PEC (between 2 and 6 mg PEC/g of fiber) was sufficient to produce flocculation. Under dynamic conditions, an increase in viscosity indicates flocculation at this low PEC dosage. Finally, under static conditions, maximum floc sizes were observed at the same PEC dosage where minimum gel points were reached. Higher PEC doses were required for CNF suspensions than for CMF suspensions.

Beeswax is a bio-sourced, renewable, and even edible material that stands as a convincing option to provide paper-based food packaging with moisture resistance. Nonetheless, the difficulty of dispersing it in water limits its applicability. This work uses oxidized, negatively charged cellulose nanofibers along with glycerol to stabilize beeswax-in-water emulsions above the melting point of the wax. The synergistic effects of nanocellulose and glycerol granted the stability of the dispersion even when it cooled down, but only if the concentration of nanofibers was high enough. This required concentration (0.6–0.9 wt%) depended on the degree of oxidation of the cellulose nanofibers. Rheological hindrance was essential to prevent the buoyancy of beeswax particles, while the presence of glycerol prevented excessive aggregation. The mixtures had yield stress and showed pseudoplastic behavior at a high enough shear rate, with their apparent viscosity being positively influenced by the surface charge density of the nanofibers. When applied to packaging paper, the nanocellulose-stabilized beeswax suspensions not only enhanced its barrier properties towards liquid water (reaching a contact angle of 96°) and water vapor (−2 d−1), but also to grease (Kit rating: 5) and airflow (>1400 Gurley s). While falling short of polyethylene-coated paper, this overall improvement, attained using only one layer of a biobased coating suspension, should be understood as a step towards replacing synthetic waxes and plastic laminates.

Composite materials containing natural reinforcement fibers, generally called biocomposites, have attracted the interest of both researchers and manufacturers, but the most environmentally advantageous combinations include a bio-based matrix, as well. With this in mind, a poly(lactic acid) (PLA) matrix was reinforced with natural fibers from hemp, both untreated strands (UHSs) and soda-bleached fibers (SBHFs). The preparation of the subsequent fully bio-sourced, discontinuously reinforced composites involved kinetic mixing, intensive single-screw extrusion, milling, and injection molding. Up to a fiber content of 30 wt%, the tensile modulus increased linearly with the volume fraction of the dispersed phase. Differences between SBHFs (up to 7.6 Gpa) and UHSs (up to 6.9 Gpa) were hardly significant (p = 0.1), but SBHF-reinforced composites displayed higher strain at failure. In any case, for the same fiber load (30 wt%), the Young’s modulus of PLA/hemp biocomposites was greater than that of glass fiber (GF)-reinforced polypropylene (5.7 GPa), albeit lower than that of PLA/GF (9.8 GPa). Considering all the measurements, the contribution of each phase was analyzed by applying the Hirsch model and the Tsai-Pagano model. As a concluding remark, although the intrinsic tensile modulus of SBHFs was lower than that of GF, the efficiency of those natural fibers as reinforcement (according to the rule of mixtures) was found to be higher.

Bio-based polymers, with any of their constituents based on nonrenewable sources, can answer the demands of society and regulations regarding minimizing the environmental impact. The more similar such biocomposites are to oil-based composites, the easier the transition, especially for companies that do not like the uncertainty. A BioPE matrix, with a structure similar to that of a high-density polyethylene (HDPE), was used to obtain abaca-fiber-reinforced composites. The tensile properties of these composites are displayed and compared with commercial glass-fiber-reinforced HDPE. Since the strength of the interface between the reinforcements and the matrix is responsible for the exploitation of the strengthening abilities of the reinforcements, several micromechanical models were used to obtain an estimation of the strength of the interface and the intrinsic tensile strength of the reinforcements. Biocomposites require the use of a coupling agent to strengthen their interface, and once an 8 wt.% of such coupling agent was added to the composites, these materials returned tensile properties in line with commercial glass-fiber-reinforced HDPE composites.

The international research community has made significant efforts in the production, characterization, and application of cellulose nanofibers (CNFs) in many sectors [...]

The use of bio-based matrices together with natural fibers as reinforcement is a strategy for obtaining materials with competitive mechanical properties, costs, and environmental impacts. However, bio-based matrices, unknown by the industry, can be a market entry barrier. The use of bio-polyethylene, which has properties similar to polyethylene, can overcome that barrier. In this study, composites reinforced with abaca fibers used as reinforcement for bio-polyethylene and high density polyethylene are prepared and tensile tested. A micromechanics analysis is deployed to measure the contributions of the matrices and reinforcements and to measure the evolution of these contributions regarding AF content and matrix nature. The results show that the mechanical properties of the composites with bio-polyethylene as a matrix were slightly higher than those of the composites with polyethylene as a matrix. It was also found that the contribution of the fibers to the Young’s moduli of the composites was susceptible to the percentage of reinforcement and the nature of the matrices. The results show that it is possible to obtain fully bio-based composites with mechanical properties similar to those of partially bio-based polyolefin or even some forms of glass fiber-reinforced polyolefin.

Composites from polypropylene (PP) reinforced with hemp strands (HS) are prepared in the current work with the aim of deepening on the influence of this reinforcement on the impact performance of these specific composites. Despite all the research conducted in this field, the effect of this natural reinforcement on the absorbed energy during crack formation and propagation is not fully tackled in previous research works. From the methodology and samples’ geometry, the results concluded that the quality of the interface has a noticeable role in the impact resistance of these materials. The interface strength, fiber dispersion and fiber pullout are the main contributors to crack formation, whereas fiber pullout is the main one responsible for crack propagation. Maximum values of absorbed energy were found for PP composites comprising 20–30 wt% of HS and 8 wt% of the coupling agent for the un-notched samples, whereas maximum absorbed energy values corresponded to PP composites with 40 wt% of HS and 4 wt% of coupling agent for the notched samples. The water-absorption behavior in different humid environments is also examined. From the kinetic study, the water diffusion followed a Fickean behavior showing low-diffusion coefficients, increasing with fiber content. This systematic investigation represents a contribution to the analysis of the potential of reinforcing conventional polymers with natural materials, as a strategy towards more sustainable development.

In this study, tensile properties of abaca-reinforced HDPE and BioPE composites have been researched. The strength of the interface between the matrix and the reinforcement of a composite material noticeably impacts its mechanical properties. Thus, the strength of the interface between the reinforcements and the matrices has been studied using micromechanics models. Natural fibers are hydrophilic and the matrices are hydrophobic, resulting in weak interfaces. In the study, a coupling agent based on polyethylene functionalised with maleic acid was used, to increase the strength of the interface. The results show that 8 wt% coupling agent contents noticeably increased the tensile strength of the composites and the interface. Tensile properties obtained for HDPE and BioPE-based coupled composites were statistically similar or better for BioPE-based materials. The use of bio-based matrices increases the possibility of decreasing the environmental impact of the materials, obtaining fully bio-based composites. The article shows the ability of fully bio-based composites to replace others using oil-based matrices.

Lignin-containing cellulose nanofibrils (LCNFs) have emerged as a new class of nanocelluloses where the presence of residual lignin is expected to impart additional attributes such as hydrophobicity or UV-absorption. In the present work, LCNFs with a lignin content between 7 and 15 wt% were prepared via a TEMPO-mediated oxidation as chemical pretreatment followed by high-pressure homogenization. The impact of the carboxyl content (CC) on the properties of the resulting LCNF gel, in terms of lignin content, colloidal properties, morphology, crystallinity, and thermal stability, were investigated. It was found that lignin content was significantly decreased at increasing CC. In addition, CC had a positive effect on colloidal stability and water contact angle, as well as resulting in smaller fibrils. This lower size, together with the lower lignin content, resulted in a slightly lower thermal stability. The reinforcing potential of the LCNFs when incorporated into a ductile polymer matrix was also explored by preparing nanocomposite films with different LCNF contents that were mechanically tested under linear and non-linear regimes by dynamic mechanical analysis (DMA) and tensile tests. For comparison purposes, the reinforcing effect of the LCNFs with lignin-free CNFs was also reported based on literature data. It was found that lignin hinders the network-forming capacity of LCNFs, as literature data shows a higher reinforcing potential of lignin-free CNFs. Nonetheless, the tensile strength of the acrylic matrix was enhanced by 10-fold at 10 wt% of LCNF content.

The compatibility between poly(lactic acid) (PLA) and natural fibers to develop bio-sourced, recyclable, and biodegradable composites remains a commonplace issue. This work highlights that, at least in the case of hemp, pulping and bleaching towards delignified short fibers attained remarkable improvements over untreated hemp strands. This approach differs from usual proposals of chemically modifying hydroxyl groups. Soda-bleached hemp fibers (SBHFs) granted a relatively large bonding surface area and a satisfactory quality of the interphase, even in the absence of any dispersant or compatibilizer. To attain satisfactory dispersion, the matrix and the fibers were subjected to kinetic mixing and to a moderately intensified extrusion process. Then, dog-bone specimens were prepared by injection molding. Up to a fiber content of 30 wt.%, the tensile strength increased linearly with the volume fraction of the dispersed phase. It reached a maximum value of 77.8 MPa, signifying a relative enhancement of about 52%. In comparison, the tensile strength for PLA/hemp strands was 55.7 MPa. Thence, based on the modified rule of mixtures and the Kelly & Tyson modified equation, we analyzed this performance at the level of the constituent materials. The interfacial shear strength (over 28 MPa) and other micromechanical parameters were computed. Overall, this biocomposite was found to outperform a polypropylene/sized glass fiber composite (without coupling agent) in terms of tensile strength, while fulfilling the principles of green chemistry.

Mater-Bi® is one of the most commercialized starch-based blends used in biodegradable flexible packaging. However, the high ductility and low stiffness of Mater-Bi® might limit its application and developing a solution to tailor the stiffness and mechanical strength is highly desirable. In the present work, blends based on Mater-Bi® and poly-L-(lactic acid) (PLLA) at a different ratio from 70/30 to 50/50 wt% were prepared via melt-extrusion and the effect of the PLLA content and Joncryl ADR® as a reactive compatibilizing agent, on the mechanical properties, melts rheology, morphology and disintegration aptitude were investigated. The inclusion of PLLA in Mater-Bi® has a marked beneficial effect on the tensile strength and stiffness of the blend while maintaining acceptable ductility. The addition of the reactive compatibilizing agent contributed to improving the strength and elongation at the break of the blend. The melt rheology of the blend was also affected by the ratio of the two components, mostly when the Joncryl ADR® was present. The disintegration by biodegradation of the blend was preserved in the presence of PLLA, and it takes less than 30 days for the films to completely decompose and disintegrate under controlled composting conditions. Interestingly, a thin film from Mater-Bi®/PLLA 60/40 was successfully prepared by blown film extrusion, demonstrating a good balance between stretchability (elongation at break exceeding 100%) and stiffness (1.8 GPa). This work opened to broadening the use of starch-based biodegradable plastic toward more demanding applications such as mulching films.

Measurements of nanocellulose size usually demand very high-resolution techniques and tedious image processing, mainly in what pertains to the length of nanofibers. Aiming to ease the process, this work assesses a relatively simple method to estimate the dimensions of nanocellulose particles with an aspect ratio greater than 1. Nanocellulose suspensions, both as nanofibers and as nanocrystals, are subjected to dynamic light scattering (DLS) and to field-emission scanning electron microscopy (FE-SEM). The former provides the hydrodynamic diameter, as long as the scatter angle and the consistency are adequate. Assays with different angles and concentrations compel us to recommend forward scattering (12.8°) and concentrations around 0.05–0.10 wt %. Then, FE-SEM with magnifications of ×5000–×20,000 generally suffices to obtain an acceptable approximation for the actual diameter, at least for bundles. Finally, length can be estimated by a simple geometric relationship. Regardless of whether they are collected from FE-SEM or DLS, size distributions are generally skewed to lower diameters. Width distributions from FE-SEM, in particular, are well fitted to log-normal functions. Overall, while this method is not valid for the thinnest fibrils or for single, small nanocrystals, it can be useful in lieu of very high-resolution techniques.

The development of new materials is currently focused on replacing fossil-based plastics with sustainable materials. Obtaining new bioplastics that are biodegradable and of the greenest possible origin could be a great alternative for the future. However, there are some limitations—such as price, physical properties, and mechanical properties—of these bioplastics. In this sense, the present work aims to explore the potential of lignin present in black liquor from paper pulp production as the main component of a new plastic matrix. For this purpose, we have studied the simple recovery of this lignin using acid precipitation, its thermoplastification with glycerin as a plasticizing agent, the production of blends with poly(caprolactone) (PCL), and finally the development of biocomposite materials reinforcing the blend of thermoplastic lignin and PCL with stone groundwood fibers (SGW). The results obtained show that thermoplastic lignin alone cannot be used as a bioplastic. However, its combination with PCL provided a tensile strength of, e.g., 5.24 MPa in the case of a 50 wt.% blend. In addition, when studying the properties of the composite materials, it was found that the tensile strength of a blend with 20 wt.% PCL increased from 1.7 to 11.2 MPa with 40 wt.% SGW. Finally, it was proven that through these biocomposites it is possible to obtain a correct fiber–blend interface.

Food packaging manufacturers often resort to lamination, typically with materials which are neither non-biodegradable nor biobased polymers, to confer barrier properties to paper and cardboard. The present work considers a greener solution: enhancing paper’s resistance to moisture, grease, and air by aqueous coating suspensions. For hydrophobization, a combined approach between nanocellulose and common esterifying agents was considered, but the water vapor transmission rate (WVTR) remained excessively high for the goal of wrapping moisture-sensitive products (>600 g m−2 d−1). Nonetheless, oil-repellant surfaces were effectively obtained with nanocellulose, illite, sodium alginate, and/or poly(vinyl alcohol) (PVA), reaching Kit ratings up to 11. Regarding air resistance, mineral-rich coatings attained values above 1000 Gurley s. In light of these results, nanocellulose, minerals, PVA, pullulan, alginate, and a non-ionic surfactant were combined for multi-purpose coating formulations. It is hypothesized that these materials decrease porosity while complementing each other’s flaws, e.g., PVA succeeds at decreasing porosity but has low dimensional stability. As an example, a suspension mostly constituted by nanocellulose, sizing agents, minerals and PVA yielded a WVTR of roughly 100 g m−2 d−1, a Kit rating of 12, and an air resistance above 300 s/100 mL. This indicates that multi-purpose coatings can be satisfactorily incorporated into paper structures for food packaging applications, although not as the food contact layer.

The current need to develop more sustainable processes and products requires the study of new materials. In the field of plastic materials, the need to develop 100% bio-based materials that meet market requirements is evident. In this sense, the present work aims to explore the potential of rapeseed waste as a reinforcement of a bio-based plastic matrix that does not generate new sub-waste. For this purpose, three types of processing of rapeseed residues have been studied: (i) milling; (ii) mechanical process; (iii) thermomechanical process. In addition, the reinforcing capacity of these materials, together with the need for an optimized coupling agent at 6 wt.%, has been verified. The micromechanics of the materials have been evaluated to determine the development of these fibers in the composite material. The results obtained show remarkable increases in mechanical properties, reaching more than 141% in tensile strength and 128% in flexural strength. There is a remarkable difference in the impact behavior between the materials with milled rapeseed and the fibers obtained by mechanical or thermomechanical processes. It was found that by sustainable design it is possible to achieve a 76.2% reduction in the amount of plastic used to manufacture material with the same mechanical properties.

The current trends in micro-/nanofibers offer a new and unmissable chance for the recovery of cellulose from non-woody crops. This work assesses a technically feasible approach for the production of micro- and nanofibrillated cellulose (MNFC) from jute, sisal and hemp, involving refining and enzymatic hydrolysis as pretreatments. Regarding the latter, only slight enhancements of nanofibrillation, transparency and specific surface area were recorded when increasing the dose of endoglucanases from 80 to 240 mg/kg. This supports the idea that highly ordered cellulose structures near the fiber wall are resistant to hydrolysis and hinder the diffusion of glucanases. Mechanical MNFC displayed the highest aspect ratio, up to 228 for hemp. Increasing the number of homogenization cycles increased the apparent viscosity in most cases, up to 0.14 Pa·s at 100 s−1 (1 wt.% consistency). A shear-thinning behavior, more marked for MNFC from jute and sisal, was evidenced in all cases. We conclude that, since both the raw material and the pretreatment play a major role, the unique characteristics of non-woody MNFC, either mechanical or enzymatically pretreated (low dose), make it worth considering for large-scale processes.

While the potential of cellulose nanofibers to enhance the mechanical and barrier properties of paper is well-known, there are many uncertainties with respect to how to apply them. In this study, we use not only bulk addition of micro-/nanofibers and bar coating with oxidized nanofibers, but also a combination of these and, as a novel element, electrospray deposition of nanofiber dispersions. Characterization involved testing the strength of uncoated and coated paper sheets, their resistance to air flow, their Bendtsen roughness, and their apparent density, plus visualization of their surface and cross-sections by scanning electron microscopy. As expected, bulk addition to the unrefined pulp was sufficient to attain substantial strengthening, but this enhancement was limited to approximately 124%. Following this, surface addition by bar coating improved air resistance, but not strength, since, as applying nanocellulose at high consistency was technically unfeasible, this was performed several times with detrimental drying stages in between. However, replacing bar coating with electrospraying helped us overcome these apparent limitations, producing enhancements in both barrier and tensile properties. It is concluded that electrosprayed nanofibers, owing to their uniform deposition and favorable interactions, operate as an effective binder between fibers (and/or fines).

In this study, Young’s modulus of henequen fibers was estimated through micromechanical modeling of polypropylene (PP)-based composites, and further corroborated through a single filament tensile test after applying a correction method. PP and henequen strands, chopped to 1 mm length, were mixed in the presence of maleic anhydride grafted polypropylene (MAPP). A 4 wt.% of MAPP showed an effective enhancement of the interfacial adhesion. The composites were mold-injected into dog-bone specimens and tensile tested. The Young’s modulus of the composites increased steadily and linearly up to 50 wt.% of fiber content from 1.5 to 6.4 GPa, corresponding to a 327% increase. Certainly, henequen fibers showed a comparable stiffening capacity of PP composites than glass fibers. The intrinsic Young’s modulus of the fibers was predicted through well established models such as Hirsch or Tsai-Pagano, yielding average values of 30.5 and 34.6 GPa, respectively. The single filament test performed to henequen strands resulted in values between 16 and 27 GPa depending on the gauge length, although, after applying a correction method, a Young’s modulus of 33.3 GPa was obtained. Overall, the present work presents the great potential for henequen fibers as PP reinforcement. Moreover, relationships between micromechanics models and filament testing to estimate Young’s modulus of the fibers were explored.

Leather waste (BF) and high-density polyethylene (HDPE) were compounded in a lab scale internal mixer and processed by means of injection molding. In this study, leather waste and HDPE composites were characterized by instrumental techniques such as differential scanning calorimetry (DSC), thermo-gravimetric Analysis (TGA), and Fourier transform infrared spectroscopy (FTIR). Physical integrity of composites against chemical exposure and chromium-leaching properties of the composites were also investigated. This study shows that the incorporation of 30% leather waste fiber into HDPE composites decreases the thermal conductivity of the composite samples by 17% in comparison to that of neat HDPE samples. Composites showed no thermal degradation during processing cycle. Strong interfacial bonding between leather waste and polymer results in comparable low-leachate levels to maximum allowed concentration for nonhazardous waste, and good chemical resistance properties. The BF/HDPE composites could be a promising low-cost alternative in industrial application areas of HDPE, where high-mechanical strength and low-thermal conductivity is required.

Noise pollution has been identified as a cause of a broad spectrum of diseases, motivating researchers to identify building materials capable of attenuating this pollution. The most common solution is the use of gypsum boards, which show a good response for low frequencies but have a poorer response for high frequencies. In addition, due to environmental concerns associated with buildings, the use of materials that minimize environmental impacts must be favored. In this research, two biopolymers, a poly(lactic) acid and a bio-polyethylene, were filled with two typologies of calcium carbonate, and their soundproofing properties were tested using impedance tubes. In addition, the morphology of the fillers was characterized, and here we discuss its impact on the mechanical properties of the composites. The results showed that the incorporation of calcium carbonate into bio-based thermoplastic materials can represent a strong alternative to gypsum, because their mechanical properties and sound barrier performance are superior. In addition, the inclusion of mineral fillers in thermoplastic materials has a positive impact on production costs, in addition to preserving the advantages of thermoplastics in terms of processing and recycling. Although the use of carbonate calcium decreases the mechanical properties of the materials, it enables the production of materials with insulation that is four-fold higher than that of gypsum. This demonstrates the potential of these materials as building lightweight solutions.

The present paper proposes a novel approach for the morphological characterization of cellulose nano and microfibers suspensions (CMF/CNFs) based on the analysis of eroded CMF/CNF microscopy images. This approach offers a detailed morphological characterization and quantification of the micro and nanofibers networks present in the product, which allows the mode of fibrillation associated to the different CMF/CNF extraction conditions to be discerned. This information is needed to control CMF/CNF quality during industrial production. Five cellulose raw materials, from wood and non-wood sources, were subjected to mechanical, enzymatic, and (2,2,6,6-Tetramethylpiperidin-1-yl)oxyl (TEMPO)-mediated oxidative pre-treatments followed by different homogenization sequences to obtain products of different morphologies. Skeleton analysis of microscopy images provided in-depth morphological information of CMF/CNFs that, complemented with aspect ratio information, estimated from gel point data, allowed the quantification of: (i) fibers peeling after mechanical pretreatment; (ii) fibers shortening induced by enzymes, and (iii) CMF/CNF entanglement from TEMPO-mediated oxidation. Being mostly based on optical microscopy and image analysis, the present method is easy to implement at industrial scale as a tool to monitor and control CMF/CNF quality and homogeneity.

The textile sector produces yearly great quantities of cotton byproducts, and the major part is either incinerated or landfilled, resulting in serious environmental risks. The use of such byproducts in the composite sector presents an attractive opportunity to valorize the residue, reduce its environmental impact, and decrease the pressure on natural and synthetic resources. In this work, composite materials based on polypropylene and dyed cotton byproducts from the textile industry were manufactured. The competitiveness of the resulting composites was evaluated from the analyses, at macro and micro scales, of the flexural modulus. It was observed that the presence of dyes in cotton fibers, also a byproduct from the production of denim items, notably favored the dispersion of the phases in comparison with other cellulose-rich fibers. Further, the presence of a coupling agent, in this case, maleic anhydride grafted polypropylene, enhanced the interfacial adhesion of the composite. As a result, the flexural modulus of the composite at 50 wt.% of cotton fibers enhanced by 272% the modulus of the matrix. From the micromechanics analysis, using the Hirsch model, the intrinsic flexural modulus of cotton fibers was set at 20.9 GPa. Other relevant micromechanics factors were studied to evaluate the contribution and efficiency of the fibers to the flexural modulus of the composite. Overall, the work sheds light on the potential of cotton industry byproducts to contribute to a circular economy.

In this work, date palm waste (DPW) stemming from the annual pruning of date palm was used as a reinforcing filler in polypropylene matrix at 20–60 wt.%. Only a grinding process of the DPW has been performed to ensure no residue generation and full utilization. The present work investigates how the DPW use affects mechanical properties and water absorption of the ensuing composite. The effect of the addition of maleated polypropylene (MAPP) as a coupling agent on the composite properties was also studied. It was shown that the reinforcing potential of DPW was strongly dependent on aspect ratio and interface quality. The MAPP addition resulted in a composite with higher strength and stiffness than the neat PP, meaning that DPW behaves as reinforcement. The difference in the reinforcing effect was explained by the change in the quality of the interface between date palm waste and the polypropylene polymeric chain.

Ultrasonic molding (USM) is a good candidate for studying the plasticization of polymer mixtures or other composite materials due to either the little amount of material needed for processing, low waste or the needed low pressure and residence time of the mold. Thus, the novelty of this research is the capability of USM technology to process PLA/PCL blends and their corresponding neat materials, encompassing all the production stages, from raw material to the final specimen. The major findings of the work revealed that the thermal properties of the blends were not affected by the USM process, although the crystallinity degree experienced variations, decreasing for PLA and increasing for PCL, which was attributed to the crystallization rate of each polymer, the high process speed, the short cooling time and the small particle size. The employed ultrasonic energy increased the molecular weight with low variations through the specimen. However, the degradation results aligned with the expected trend of these material blends. Moreover, this study also showed the effect pellet shape and dimensions have over the process parameters, as well as the effect of the blend composition. It can be concluded that USM is a technology suitable to successfully process PLA/PCL blends with the correct determination of process parameter windows.

In this study, experimental analysis on the compressive strength of multi-leaf thin-tile masonry is presented. A compressive strength test was carried out on thin-tile, mortar and 48 specimens with two- and three-leaf thin-tile masonry. The results obtained were compared with literature on brick masonry loaded parallel to a bed joint. Based on the results of this study, the failure mode presented the first crack in the vertical interface; this crack grew until the leaf was detached. From this point until collapse, lateral buckling of the leaves was generally observed. Therefore, the detachment compressive strength value was considered relevant. Up to this point, both masonries exhibit similar stress–strain behavior. The experimental values of the detachment compressive strength were compared with the values calculated from the equation generally used in the literature to evaluate the compressive strength of brick masonry. From the results obtained, the following conclusion can be drawn: This equation is only suitable for tree-leaf thin-tile masonry but with more relevant influence on the compressive strength of the mortar. This study concluded that only three-leaf specimens behave similarly to brick masonry loaded parallel to a bed joint. Finally, whether the failure mode was due to shear or tensile stresses in the vertical thin-tile-mortar interface cannot be identified.

Date palm waste is an abundant agricultural residue in Tunisia and can be used for plastic reinforcement. Moreover, its use in plastic composites can help to reduce dependence on fossil resources for material production. In this work, the valorization of date palm residues was studied by employing high-yield processes following mechanical, chemical, and enzymatical treatments. Fibers obtained by soft chemical treatment with sodium hydroxide and enzymatic treatment with xylanases and pectinases were evaluated for their use in the reinforcement of plastic materials. The flexural strength property, truly relevant for structural, construction, automotive, or other market sectors, was adopted to assess the reinforcing potential of the fibers. Polypropylene was effectively reinforced with date palm fibers (60 wt.%), exhibiting a flexural strength increases of 80% (73.1 MPa), 93% (78.5 MPa), and 106% (83.9 MPa) for mechanical, chemical, and enzymatic fibers, respectively. The different treatments had an impact on the chemical composition of the fibers, and by extension on the final properties of the composites. The holocellulose content could provide good interfacial adhesion using a coupling agent, whereas the lignin content improved the dispersion of the phases. Two interesting outcomes were that the flexural performance of enzymatic fibers was like that of wood composites, whereas the specific flexural strength was comparable to that of glass fiber composites. Overall, the present work has shown the potential behind date palm waste in the composite sector when a specific property or application is desired. Novel treatments have been used for greater fiber compatibility, increasing the sustainability of the process, and improving the applicability of the palm residue.

Biocomposites are composite materials where at least the matrix or the reinforcement phases are obtained from natural and renewable resources. Natural fibers for composite preparation can be obtained from annual plants, wood, recycled products, or agroforestry waste. The present work selected abaca strands, spruce fibers, recycled fibers from old newspaper, and barley fibers as raw materials to produce biocomposites, in combination with a biobased polyethylene. One very important feature in material science and for industrial applications is knowing how a material will deform under load, and this characteristic is represented by Young’s modulus. Therefore, in this work, the stiffness and deformation of the biocomposites were determined and evaluated using macromechanics and micromechanics analyses. Results were compared to those of conventional synthetic composites reinforced with glass fibers. From the micromechanics analysis, the intrinsic Young modulus of the reinforcements was obtained, as well as other micromechanics parameters such as the modulus efficiency and the length and orientation factors. Abaca strands accounted for the highest intrinsic modulus. One interesting outcome was that recycled fibers exhibited similar Young’s moduli to wood fibers. Finally, agroforestry waste demonstrated the lowest stiffening potential. The study explores the opportunity of using different natural fibers when specific properties or applications are desired.

Leather buffing dust (BF) is a waste from tannery which is usually disposed on landfills. The interest in using wastes as fillers or reinforcements for composites has raised recently due to environmental concerns. This study investigates the potential use of BF waste as filler for a high density polyethylene matrix (HDPE). A series of HDPE-BF composites, containing filler concentrations ranging from 20 to 50wt%, were formulated, injection molded and tested. The effect of filler contents on the mechanical properties of the composites were evaluated and discussed. Composites with BF contents up to 30wt% improved the tensile strength and Young’s modulus of the matrix, achieving similar mechanical properties to polypropylene (PP). In the case of flexural strength, it was found to be proportionally enhanced by increasing reinforcement content, maintaining high impact strength. These composites present great opportunities for PP application areas that require higher impact resistance. The materials were submitted to a series of closed-loop recycling cycles in order to assess their recyclability, being able to maintain better tensile strength than virgin HDPE after 5 cycles. The study develops new low-cost and sustainable composites by using a waste as composite filler.

The research toward environmentally friendly materials has devoted a great effort on composites based on natural fiber-reinforced biopolymers. These materials have shown noticeable mechanical properties, mainly tensile and flexural strengths, as a consequence of increasingly strong interfaces. Previous studies have shown a good interface between natural fibers and poly (lactic acid) (PLA) when these fibers present a low lignin content in their surface chemical composition (bleached fibers). Nonetheless, one of the main drawbacks of these materials is the hydrophilicity of the reinforcements in front of the mineral ones like glass fiber. Meanwhile, the behavior of such materials under impact is also of importance to evaluate its usefulness. This research evaluates the water uptake behavior and the impact strength of bleached Kraft softwood-reinforced PLA composites that have been reported to show noticeable tensile and flexural properties. The paper explores the differences between these bio-based materials and commodity composites like glass fiber-reinforced polypropylene.

The present work aims at determining the potential of date palm wastes to be applied as reinforcement in polypropylene. For this, fibers were separated from the raw biomass via mechanical defibration in Sprout Waldron equipment. Then, three different treatment strategies were adopted on the fibers, being (i) mechanical, (ii) chemical with NaOH, and (iii) enzymatical with xylanases and pectinases. Fibers were characterized in terms of chemical composition, morphology and SEM. Additionally, PP was reinforced with date palm fibers and the composites’ stiffness was evaluated. The analysis was performed from a macro and micro mechanical viewpoint. The incorporation of 40 and 60 wt.% of DPF-E enhanced the Young’s modulus of PP by 205 and 308%, respectively. The potential of enzymatically treated fibers to replace glass fibers in composites was studied, exhibiting similar stiffening abilities at 60 wt.% of date palm fiber (6.48 GPa) and 40% of glass fibers (6.85 GPa). The intrinsic Young’s modulus of the fibers was set at values around 16, 20 and 24 GPa for mechanical, chemical and enzymatic fibers. From the micromechanical analysis, the efficiency of the reinforcement as well as the contribution of the length and orientation to the Young’s modulus of the composite was evaluated.

In this work, date palm waste (DPW) stemming from the annual pruning of date palm was used as reinforcing filler in polypropylene (PP) matrix at 40% w/w. Three pre-treatment routes were performed for the DPW, namely (i) defibration, (ii) soft alkali treatment, and (iii) enzymatic treatment, to obtain date palm fibers (DPF) and to investigate the effect of each process on their chemical composition, which will ultimately affect the mechanical properties of the resulting composites. The enzymatic and alkali treatment, combined with maleated polypropylene (MAPP) as a coupling agent, resulted in a composite with higher strength and stiffness than the neat PP. The differences in the reinforcing effect were explained by the change in the morphology of DPF and their chemical surface composition according to the selected treatment of DPW. Enzymatic treatment maximized the tensile strength of the compound as a consequence of an improvement in the interfacial shear strength and the intrinsic resistance of the fibers.

Circular economy comes to break the linear resource to waste economy, by introducing different strategies, two of them being: using material from renewable sources and producing biodegradable products. The present work aims at developing polylactic acid (PLA), typically made from fermented plant starch, and polycaprolactone (PCL) blends, a biodegradable polyester, to study their potential to be used as substitutes of oil-based commodity plastics. For this, PLA/PCL blends were compounded in a batch and lab scale internal mixer and processed by means of injection molding. Tensile and impact characteristics were determined and compared to different thermoplastic materials, such as polypropylene, high density polyethylene, polystyrene, and others. It has been found that the incorporation of PCL into a PLA matrix can lead to materials in the range of 18.25 to 63.13 megapascals of tensile strength, 0.56 to 3.82 gigapascals of Young’s modulus, 12.65 to 3.27 percent of strain at maximum strength, and 35 to 2 kJ/m2 of notched impact strength. The evolution of the tensile strength fitted the Voigt and Reuss model, while Young’s modulus was successfully described by the rule of mixtures. Toughness of PLA was significantly improved with the incorporation of PCL, significantly increasing the energy required to fracture the specimens. Blends containing more than 20 wt% of PCL did not break when unnotched specimens were tested. Overall, it was found that the obtained PLA/PCL blends can constitute a strong and environmentally friendly alternative to oil-based commodity materials.

Hemp core is a lignocellulosic residue in the production chain of hemp strands. Huge amounts of hemp core are gathered annually in Europe (43,000 tons) with no major application end. Such lignocellulosic wastes have potential as filling or reinforcing material to replace synthetic fibers and wood fibers in polymer composites. In this study, hemp core biomass was treated under different NaOH concentrations and then defibrated by means of Sprout Waldron equipment to obtain single fibers. Polypropylene matrix was reinforced up to 50 wt.% and the resulting hemp core fibers and the flexural properties were investigated. The results show that the flexural strength of composites increased with the intensity of NaOH treatment. The effect of NaOH was attributed to the removal of extractives and lignin in the fiber cell wall leading to improved interfacial adhesion characteristics. Besides, a methodology was established for the estimation of the intrinsic flexural strength of hemp core fibers. The intrinsic flexural strength of hemp core fibers was calculated to be 940 MPa for fibers treated at 10 wt.% of NaOH. In addition, a relationship between the lignin content and the intrinsic strength of the fibers was established.

Automotive and industrial design companies have profusely used commodity materials like glass fiber-reinforced polypropylene. These materials show advantageous ratios between cost and mechanical properties, but poor environmental yields. Natural fibers have been tested as replacements of glass fibers, obtaining noticeable tensile strengths, but being unable to reach the strength of glass fiber-reinforced composites. In this paper, polyamide 6 is proposed as a matrix for cellulosic fiber-based composites. A variety of fibers were tensile tested, in order to evaluate the creation of a strong interphase. The results show that, with a bleached hardwood fiber-reinforced polyamide 6 composite, it is possible to obtain tensile strengths higher than glass-fiber-reinforced polyolefin. The obtained composites show the existence of a strong interphase, allowing us to take advantage of the strengthening capabilities of such cellulosic reinforcements. These materials show advantageous mechanical properties, while being recyclable and partially renewable.

The present work aims to combine the unique properties of cellulose nanofibers (CNF) with polyvinyl alcohol (PVA) to obtain high-performance nanocomposites. CNF were obtained by means of TEMPO-mediated ((2,2,6,6-Tetramethylpiperidin-1-yl)oxyl) oxidation, incorporated into the PVA matrix by means of compounding in a single-screw co-rotating internal mixer and then processed by means of injection molding. It was found that CNF were able to improve the tensile strength of PVA in 85% when 4.50 wt % of CNF were added. In addition, the incorporation of a 2.25 wt % of CNF enhanced the tensile strength to the same level that when 40 wt % of microsized fibers (stone groundwood pulp, SGW) were incorporated, which indicated that CNF possessed significantly higher intrinsic mechanical properties than microsized fibers. SGW was selected as reference for microsized fibers due to their extended use in wood plastic composites. Finally, a micromechanical analysis was performed, obtaining coupling factors near to 0.2, indicating good interphase between CNF and PVA. Overall, it was found that the use of CNF is clearly advantageous to the use of common cellulosic fibers if superior mechanical properties are desired, but there are still some limitations that are related to processing that restrict the reinforcement content at low contents.

Natural fiber-reinforced thermoplastic composites can be an alternative to mineral fiber-based composites, especially when economic and environment concerns are included under the material selection criteria. In recent years, the literature has shown how lignocellulosic fiber-reinforced composites can be used for a variety of applications. Nonetheless, the impact strength and the water uptake behavior of such materials have been seen as drawbacks. In this work, the impact strength and the water uptake of composites made of polypropylene reinforced with fibers from recycled newspaper have been researched. The results show how the impact strength decreases with the percentage of reinforcement in a similar manner to that of glass fiber-reinforced polypropylene composites as a result of adding a fragile phase to the material. It was found that the water uptake increased with the increasing percentages of lignocellulosic fibers due to the hydrophilic nature of such reinforcements. The diffusion behavior was found to be Fickian. A maleic anhydride was added as a coupling agent in order to increase the strength of the interface between the matrix and the reinforcements. It was found that the presence of such a coupling agent increased the impact strength of the composites and decreased the water uptake. Impact strengths of 21.3 kJ/m3 were obtained for a coupled composite with 30 wt % reinforcement contents, which is a value higher than that obtained for glass fiber-based materials. The obtained composites reinforced with recycled fibers showed competitive impact strength and water uptake behaviors in comparison with materials reinforced with raw lignocellulosic fibers. The article increases the knowledge on newspaper fiber-reinforced polyolefin composite properties, showing the competitiveness of waste-based materials.

The strength of the interphase between the reinforcements and the matrix has a major role in the mechanical properties of natural fiber reinforced polyolefin composites. The creation of strong interphases is hindered by the hydrophobic and hydrophilic natures of the matrix and the reinforcements, respectively. Adding coupling agents has been a common strategy to solve this problem. Nonetheless, a correct dosage of such coupling agents is important to, on the one hand guarantee strong interphases and high tensile strengths, and on the other hand ensure a full exploitation of the strengthening capabilities of the reinforcements. The paper proposes using topographic profile techniques to represent the effect of reinforcement and coupling agent contents of the strength of the interphase and the exploitation of the reinforcements. This representation allowed identifying the areas that are more or less sensitive to coupling agent content. The research also helped by finding that an excess of coupling agent had less impact than a lack of this component.

This paper is focused on the flexural properties of bleached kraft softwood fibers, bio-based, biodegradable, and a globally available reinforcement commonly used in papermaking, of reinforced polylactic acid (PLA) composites. The matrix, polylactic acid, is also a bio-based and biodegradable polymer. Flexural properties of composites incorporating percentages of reinforcement ranging from 15 to 30 wt % were measured and discussed. Another objective was to evaluate the strength of the interface between the matrix and the reinforcements, using the rule of mixtures to determine the coupling factor. Nonetheless, this rule of mixtures presents two unknowns, the coupling factor and the intrinsic flexural strength of the reinforcement. Hence, applying a ratio between the tensile and flexural intrinsic strengths and a defined fiber tensile and flexural strength factors, derived from the rule of mixtures is proposed. The literature lacks a precise evaluation of the intrinsic tensile strength of the reinforcements. In order to obtain such intrinsic tensile strength, we used the Kelly and Tyson modified equation as well as the solution provided by Bowyer and Bader. Finally, we were able to characterize the intrinsic flexural strengths of the fibers when used as reinforcement of polylactic acid.

Single-use plastics are expected to disappear, mainly due to the rise of stricter regulations to combat their impact on the environment. As an example, the recent European Directive on Single-Use-Plastics (SUP) will be implemented between 2021 and 2024 and will directly prohibit the use of some SUP. Baby diapers are one of the most used single-used products in our daily lives, and it is estimated that most of the ~4000 diapers that each baby uses in their life go to landfill. Such diapers usually contain superabsorbent polymers (SAP) that are based on acrylic acid-acrylamide mixtures with high water retention capacity, but they are neither bio-based nor biodegradable. In this work, we have developed bio-based superabsorbent aerogels made of cellulose nanofibers (CNF) and propose their potential use in baby diapers. TEMPO-oxidized CNF at different oxidation degrees were prepared and tested. The obtained CNF exhibited higher free swelling capacity (FSC) than the commercial fluff pulp (ranging from 117.62% to 245.21% higher) and also than the diaper absorbent, except for CNF-5 (ranging from 31.56% to 54.55%), even under compression. Overall, the present work shows a case study where CNF could have a potential application with market opportunities.

Newspapers have a limited lifespan, and therefore represent a focus of used and disposed paper. While these refuses have a considerable value and can be easily recycled, a considerable fraction ends in landfill. The authors show the possibility of adding value to used newspaper and enlarge its value chain. Old newspaper incorporates a high amount of wood fibers able to be used as reinforcement. On the other hand, this material also incorporates inks and other components inherent to newspaper production. In this work, the authors disintegrate old newspaper to recover and individualize wood fibers. A morphological analysis showed that the recovered fibers had aspect ratios higher than 10, revealing, a priori, their strengthening capabilities. Thereupon, these fibers were compounded with polypropylene at different contents, ranging from 20% to 50% w/w. It is well known that wood fibers are hydrophilic, while polyolefin are hydrophobic. This is a drawback to obtaining strong interfaces. Thus, two sets of composites were produced, with and without a coupling agent. The results showed that uncoupled composites increased the flexural strength of the matrix but reached an equilibrium point from which adding more reinforcement did not changer the flexural strength. On the other hand, the coupled composites showed a linear increase of the flexural strength against the reinforcement content. The flexural moduli of the coupled and uncoupled composites were very similar and evolved linearly with the reinforcement content.

Due to its high biocompatibility, bio-degradability, and low cost, cellulose finds application in disparate areas of research. Here we focus our attention on the potential applications of cellulose nanofiber in cement-based materials for the building sector. We first describe the chemical/morphological composition of cellulose fibers, their process and treatment, the characterization of cement-based composites, and their flexural strength. In recent research in this field, cellulose has been considered in the form of nano-sized particles, i.e., cellulose nanofibers (CNF) or cellulose nanocrystals (CNC). CNF and CNC are used for several reasons, including their mechanical and thermal properties, their extended surface area and low toxicity. This study presents some potential applications of lignocellulosic micro/nanofibers (LCMNF) in cement-based composites in order to improve flexural strength. Samples were made with 0.5-1.0-1.5-2.0 wt% of LCMNF obtained from pine sawdust, CEM I (Portland) and a 1:3 cement-water ratio. The composites were then tested for flexural strength at 7, 14, and 28 days and the evolution of flexural strength was assessed after water immersion during 72 h. Scanning electron microscopy was employed to visualize the bond between LCMNF and the cement matrix. Results showed that LCMNF improved the flexural strength of the composite in all the dosages used.

Poly(lactic acid) (PLA) is one of the most well-known biopolymers. PLA is bio-based, biocompatible, biodegradable, and easy to produce. This polymer has been used to create natural fiber reinforced composites. However, to produce high-performance and presumably biodegradable composites, the interphase between PLA and natural fibers still requires further study. As such, we aimed to produce PLA-based composites reinforced with a commercial bleached kraft eucalyptus pulp. To become a real alternative, fully biodegradable composites must have similar properties to commercial materials. The results found in this research support the competence of wood fiber reinforced PLA composites to replace other glass fiber reinforced polypropylene composites from a tensile property point of view. Furthermore, the micromechanics analysis showed that obtaining strong interphases between the PLA and the reinforcement is possible without using any coupling agent. This work shows the ability of totally bio-based composites that fulfill the principles of green chemistry to replace composites based on polyolefin and high contents of glass fiber. To the best knowledge of the authors, previous studies obtaining such properties or lower ones involved the use of reagents or the modification of the fiber surfaces’.

Cellulose nanofibers (CNF) are interesting biopolymers that find numerous applications in different scientific and technological fields. However, manufacturing costs are still one of the main drawbacks for the industrial production of highly fibrillated, transparent CNF suspensions. In the present study, cellulose nanofibers were produced from bleached eucalyptus pulp via TEMPO-mediated oxidation with varying amounts of NaClO and passed through a high-pressure homogenizer. The CNFs were chemically and physically characterized; cellulose nanopapers were also produced to study tensile properties. Production costs were also calculated. Results indicated that CNF properties are strongly dependent on the carboxyl content. Manufacturing costs showed that chemicals, in particular TEMPO catalyst, represent a large part of the final cost of CNFs. In order to solve this problem, a set of samples were prepared where the amount of TEMPO was gradually reduced. Characterization of samples prepared in this way showed that not only were the costs reduced, but also that the final properties of the CNFs were not significantly affected when the amount of TEMPO was reduced to half.