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The rational valorization of lignin and its derivatives is a challenge in biorefinery because this biopolymer is one of the major source of aromatic moieties. Lignosulfonates are used to a lesser extent than lignin to prepare macromolecular materials. In the current study, sodium lignosulfonate (NaLS), which was either blended or not blended with OH-containing vegetable oil (i.e., castor oil (CO)), was reacted with diphenylmethane diisocyanate (MDI) to prepare polyurethane-type materials, such as lignopolyurethanes (i.e., CO/NaLS/MDI and NaLS/MDI, respectively). NaLS was oxypropylated (LS-Oxy) to increase its reactivity towards MDI. LS-Oxy was characterized and then used after being blended or not blended with CO to prepare lignopolyurethanes CO/LS-Oxy/MDI and LS-Oxy/MDI, respectively. These materials were characterized by infrared spectroscopy, thermogravimetry (TG), and dynamic mechanical thermoanalysis (DMA). The Tg values obtained from DMA (loss modulus peak) indicated that the lignopolyurethanes with an intermediate degree of cross-linking were obtained. In a final set of experiments and due to their potential application, the obtained lignopolyurethanes were reinforced with sisal fibers, and the impact strength, flexural properties and scanning electron microscopy (SEM) images of the materials were obtained. The results indicated that the presence of sisal fibers led to a significant improvement in the impact strength of the lignopolyurethanes, especially in those prepared from LS-Oxy [CO/LS-Oxy/MDI: approximately from 40 J m −1 (without sisal) to 370 J m −1 (with sisal); LS-Oxy/MDI: from 15 J m −1 (without sisal) to 459 J m −1 (with sisal)]. The flexural properties of CO/LS-Oxy/MDI (with or without sisal) corresponded to a less rigid material compared to the other material. The results indicated that the characteristics of the lignopolyurethanes could be tuned by oxypropylation of NaLS and/or blending with CO as well as by the addition of sisal fibers, which enables the production of materials with a wide range of properties.

A tannin–phenolic resin (40 wt% of tannin, characterized by 1 H nuclear magnetic resonance (NMR) and 13 C NMR, Fourier transform infrared, thermogravimetry, differential scanning calorimetry) was used to prepare composites reinforced with sisal fibers (30–70 wt%). Inverse gas chromatography results showed that the sisal fibers and the tannin–phenolic thermoset have close values of the dispersive component and also have predominance of acid sites (acid character) at the surface, confirming the favoring of interaction between the sisal fibers and the tannin–phenolic matrix at the interface. The Izod impact strength increased up to 50 wt% of sisal fibers. This composite also showed high storage modulus, and the lower loss modulus, confirming its good fiber/matrix interface, also observed by SEM images. A composite with good properties was prepared from high content of raw material obtained from renewable sources (40 wt% of tannin substituted the phenol in the preparation of the matrix and 50 wt% of matrix was replaced by sisal fibers).

Tannin–phenolic polymers prepared using tannin, a macromolecule obtained from natural sources, were used in the preparation of composites reinforced with coir fibers. The composites based on tannin–phenolic polymers (50% (w/w) of tannin as substitute of the phenol) were prepared using the coir fibers as reinforcement (30–70% (w/w), 3.0–6.0 cm, randomly distributed). The Izod impact strength of the composites showed an improvement in this property due to the incorporation of coir fibers in the tannin–phenolic matrices. The SEM images showed excellent adhesion at the fiber/matrix interface. The coir fiber had bundles regularly spaced, which enhanced the diffusion of the resin into the fiber. In addition, the high lignin content of this fiber results in a high concentration of aromatic rings, which increased the compatibility with the matrix. The values of the diffusion coefficient of water, determined using Fick's laws, show that there was no correlation between the fiber percentage and the water diffusion. The DMTA curves showed that the storage moduli of the composites reinforced with coir fibers were considerably higher than that of the thermoset, and the increase in the proportion of fibers led to a proportional increase in the storage moduli of these materials. The biobased composites obtained have potential for non-structural applications, such as in the internal parts of automotives vehicles. To our knowledge, this is the first study on this kind of biobased composites.

The aim of the present work was to investigate the toughening of phenolic thermoset and its composites reinforced with sisal fibers, using hydroxyl-terminated polybutadiene rubber (HTPB) as both impact modifier and coupling agent. Substantial increase in the impact strength of the thermoset was achieved by the addition 10% of HTPB. Scanning electron microscopy (SEM) images of the material with 15% HTPB content revealed the formation of some rubber aggregates that reduced the efficiency of the toughening mechanism. In composites, the toughening effect was observed only when 2.5% of HTPB was added. The rubber aggregates were found located mainly at the matrix–fiber interface suggesting that HTPB could be used as coupling agent between the sisal fibers and the phenolic matrix. A composite reinforced with sisal fibers pre-impregnated with HTPB was then prepared; its SEM images showed the formation of a thin coating of HTPB on the surface of the fibers. The ability of HTBP as coupling agent between sisal fibers and phenolic matrix was then investigated by preparing a composite reinforced with sisal fibers pre-treated with HTPB. As revealed by its SEM images, the HTPB pre-treatment of the fibers resulted on the formation of a thin coating of HTPB on the surface of the fibers, which provided better compatibility between the fibers and the matrix at their interface, resulting in a material with low water absorption capacity and no loss of impact strength.

The (bio)degradation of polyolefins can be accelerated by modifying the level of crystallinity or by incorporation of carbonyl groups by adding pro-oxidants to masterbatches or through exposure to ultraviolet irradiation. In this work, we sought to improve the degradation of PP by adding cobalt, calcium or magnesium stearate to Ecoflex ® , PP or Ecoflex ® /PP blends. The effect of the pro-oxidants on biodegradability was assessed by examining the mechanical properties and fluidity of the polymers. PP had higher values for tensile strength at break and Young's modulus than Ecoflex ® , and the latter had little influence on the properties of PP in Ecoflex ® /PP blends. However, the presence of pro-oxidants (except for calcium) reduced these properties. All of the pro-oxidants enhanced the fluidity of PP, a phenomenon that facilitated polymer degradation at high temperatures.

Thermoset phenolic composites reinforced with sisal fibers were prepared to optimize the cure step. In the present study, processing parameters such as pressure, temperature, and time interval were varied to control the vaporization of the water generated as a byproduct during the crosslinking reaction. These molecules can vaporize forming voids, which in turn affect the final material properties. The set of results on impact strength revealed that the application of higher pressure before the gel point of the phenolic matrix produced composites with better properties. The SEM images showed that the cure cycle corresponding to the application of higher values of molding pressure at the gel point of the phenolic resin led to the reduction of voids in the matrix. In addition, the increase in the molding pressure during the cure step increased the resin interdiffusion. Better filling of the fiber channels decreased the possibility of water molecules diffusing through the internal spaces of the fibers. These molecules then diffused mainly through the bulk of the thermoset matrix, which led to a decrease in the water diffusion coefficient (D) at all three temperatures (25, 55 and 70 °C) considered in the experiments.