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The application of optimization techniques to improve the performance of polymer processing technologies is of great practical consequence, since it may result in significant savings of materials and energy resources, assist recycling schemes and generate products with better properties. The present review aims at identifying and discussing the most important characteristics of polymer processing optimization problems in terms of the nature of the objective function, optimization algorithm, and process modelling approach that is used to evaluate the solutions and the parameters to optimize. Taking into account the research efforts developed so far, it is shown that several optimization methodologies can be applied to polymer processing with good results, without demanding important computational requirements. Furthermore, within the field of artificial intelligence, several approaches can reach significant success. The first part of this review demonstrated the advantages of the optimization approach in polymer processing, discussed some concepts on multi-objective optimization and reported the application of optimization methodologies to single and twin screw extruders, extrusion dies and calibrators. This second part focuses on injection molding, blow molding and thermoforming technologies.

The present work reports the production and characterization of polyetheretherketone (PEEK) nanocomposite filaments incorporating carbon nanotubes (CNT) and graphite nanoplates (GnP), electrically conductive and suitable for fused deposition modeling (FDM) processing. The nanocomposites were manufactured by melt mixing and those presenting electrical conductivity near 10 S/m were selected for the production of filaments for FDM. The extruded filaments were characterized for mechanical and thermal conductivity, polymer crystallinity, thermal relaxation, nanoparticle dispersion, thermoelectric effect, and coefficient of friction. They presented electrical conductivity in the range of 1.5 to 13.1 S/m, as well as good mechanical performance and higher thermal conductivity compared to PEEK. The addition of GnP improved the composites’ melt processability, maintained the electrical conductivity at target level, and reduced the coefficient of friction by up to 60%. Finally, three-dimensional (3D) printed test specimens were produced, showing a Young’s modulus and ultimate tensile strength comparable to those of the filaments, but a lower strain at break and electrical conductivity. This was attributed to the presence of large voids in the part, revealing the need for 3D printing parameter optimization. Finally, filament production was up-scaled to kilogram scale maintaining the properties of the research-scale filaments.

Thermoplastic polyurethanes (TPUs) are remarkably versatile polymers due to the wide range of raw materials available for their synthesis, resulting in physicochemical characteristics that can be tailored according to the specific requirements of their final applications. In this study, a renewable bio-based polyol obtained from soybean oil is used for the synthesis of TPU via reactive extrusion, and the influence of the bio-based polyol on the multi-phase structure and properties of the TPU is studied. As raw materials, 4,4′-diphenylmethane (MDI), 1,4-butanediol, a fossil-based polyester polyol, and a bio-based polyol are used. The fossil-based to soybean-based polyol ratios studied are 100/0, 99/1, 95/5, 90/10, 80/20, and 50/50% by weight, respectively. The TPUs were characterized by size exclusion chromatography (SEC), gel content analysis, Fourier transform infrared spectroscopy (FTIR), differential scanning calorimetry (DSC), small-angle X-ray scattering (SAXS), dynamic mechanical analysis (DMA), and contact angle measurements. The results reveal that incorporating the renewable polyol enhances the compatibility between the rigid and flexible segments of the TPU. However, due to its high functionality, the addition of soybean-based polyol can promote cross-linking. This phenomenon reduces the density of hydrogen bonds within the material, also reducing polarity and restricting macromolecular mobility, as corroborated by higher glass transition temperature (Tg) values. Remarkably, the addition of small amounts of the bio-based polyol (up to 5 wt.% of the total polyol content) results in high-molecular-weight TPUs with lower polarity, combined with suitable processability and mechanical properties, thus broadening the range of applications and improving their sustainability.

Three-dimensional (3D) printing technology has become a popular tool to produce complex structures. It has great potential in the regenerative medicine field to produce customizable and reproducible scaffolds with high control of dimensions and porosity. This study was focused on the investigation of new biocompatible and biodegradable 3D-printed scaffolds with suitable mechanical properties to assist tendon and ligament regeneration. Polylactic acid (PLA) scaffolds were reinforced with 0.5 wt.% of functionalized graphite nanoplatelets decorated with silver nanoparticles ((f-EG)+Ag). The functionalization of graphene was carried out to strengthen the interface with the polymer. (f-EG)+Ag exhibited antibacterial properties against Staphylococcus aureus (S. aureus) and Escherichia coli (E. coli), an important feature for the healing process and prevention of bacterial infections. The scaffolds’ structure, biodegradation, and mechanical properties were assessed to confirm their suitability for tendon and ligamentregeneration. All scaffolds exhibited surface nanoroughness created during printing, which was increased by the filler presence. The wet state dynamic mechanical analysis proved that the incorporation of reinforcement led to an increase in the storage modulus, compared with neat PLA. The cytotoxicity assays using L929 fibroblasts showed that the scaffolds were biocompatible. The PLA+[(f-EG)+Ag] scaffolds were also loaded with human tendon-derived cells and showed their capability to maintain the tenogenic commitment with an increase in the gene expression of specific tendon/ligament-related markers. The results demonstrate the potential application of these new 3D-printed nanocomposite scaffolds for tendon and ligament regeneration.

Additive Manufacturing Techniques such as Fused Filament Fabrication (FFF) produce 3D parts with complex geometries directly from a computer model without the need of using molds and tools, by gradually depositing material(s), usually in layers. Due to the rapid growth of these techniques, researchers have been increasingly interested in the availability of strategies, models or data that may assist process optimization. In fact, 3D printed parts often exhibit limited mechanical performance, which is usually the result of poor bonding between adjacent filaments. In turn, the latter is influenced by the temperature field history during deposition. This study aims at evaluating the influence of the phase change from the melt to the solid state undergone by semi-crystalline polymers such as Polylactic Acid (PLA), on the heat transfer during the deposition stage. The energy equation considering solidification is solved analytically and then inserted into a MatLab® code to model cooling in FFF. The deposition and cooling of simple geometries is studied first, in order to assess the differences in cooling of amorphous and semi-crystalline polymers. Acrylonitrile Butadiene Styrene (ABS) was taken as representing an amorphous material. Then, the deposition and cooling of a realistic 3D part is investigated, and the influence of the build orientation is discussed.

Given the global economic and societal importance of the polymer industry, the continuous search for improvements in the various processing techniques is of practical primordial importance. This review evaluates the application of optimization methodologies to the main polymer processing operations. The most important characteristics related to the usage of optimization techniques, such as the nature of the objective function, the type of optimization algorithm, the modelling approach used to evaluate the solutions, and the parameters to optimize, are discussed. The aim is to identify the most important features of an optimization system for polymer processing problems and define the best procedure for each particular practical situation. For this purpose, the state of the art of the optimization methodologies usually employed is first presented, followed by an extensive review of the literature dealing with the major processing techniques, the discussion being completed by considering both the characteristics identified and the available optimization methodologies. This first part of the review focuses on extrusion, namely single and twin-screw extruders, extrusion dies, and calibrators. It is concluded that there is a set of methodologies that can be confidently applied in polymer processing with a very good performance and without the need of demanding computation requirements.

In the present study, poly(3-hydroxybutyrate-co-3-hydroxyhexanoate) [P(3HB-co-3HHx)] was reinforced with hydroxyapatite nanoparticles (nHA) to produce novel nanocomposites for potential uses in bone reconstruction. Contents of nHA in the 2.5–20 wt % range were incorporated into P(3HB-co-3HHx) by melt compounding and the resulting pellets were shaped into parts by injection molding. The addition of nHA improved the mechanical strength and the thermomechanical resistance of the microbial copolyester parts. In particular, the addition of 20 wt % of nHA increased the tensile (Et) and flexural (Ef) moduli by approximately 64% and 61%, respectively. At the highest contents, however, the nanoparticles tended to agglomerate, and the ductility, toughness, and thermal stability of the parts also declined. The P(3HB-co-3HHx) parts filled with nHA contents of up to 10 wt % matched more closely the mechanical properties of the native bone in terms of strength and ductility when compared with metal alloys and other biopolymers used in bone tissue engineering. This fact, in combination with their biocompatibility, enables the development of nanocomposite parts to be applied as low-stress implantable devices that can promote bone reconstruction and be reabsorbed into the human body.

Polyhydroxyalkanoates (PHAs) are natural polyesters which biodegrade in soils and oceans but have more than double the cost of comparable oil-based polymers. PHA downstreaming from its biomass represents 50% of its overall cost. Here, in an attempt to assist downstreaming, mastication of wet biomasses is tested as a new mechanical continuous biomass pretreatment with potential for industrial upscaling. Downstreaming conditions where both product recovery and purity are low due to the large amount of treated wet biomass (50% water) were targeted with the following process: extraction of 20 g in 100 mL solvent at 30 °C for 2 h, followed by 4.8 h digestion of 20 g in 0.3 M NaOH. Under the studied conditions, NaOH digestion was more effective than solvent extraction in recovering larger PHA amounts, but with less purity. A nearly 50% loss of PHA was seen during digestion after mastication. PHAs downstreamed by digestion with large amounts of impurities started to degrade at lower temperatures, but their melt elasticity was thermally stable at 170 °C. As such, these materials are attractive as fully PHA-compatible processing aids, reinforcing fillers or viscosity modifiers. On the other hand, wet biomass mastication before solvent extraction improves PHA purity and thermal stability as well as the melt rheology, which recovers the viscoelasticity measured with a PHA extracted from a dried biomass.

The use of real-time techniques to evaluate the global mixing performance of co-rotating twin-screw extruders is well consolidated, but much less is reported on the specific contribution of individual screw zones. This work uses on-line flow turbidity and birefringence to ascertain the mixing performance of kneading blocks with different geometries. For this purpose, one of the barrel segments of the extruder was modified in order to incorporate four sampling devices and slit dies containing optical windows were attached to them. The experiments consisted in reaching steady extrusion and then adding a small amount of tracer. Upon opening each sampling device, material was laterally detoured from the local screw channel, and its turbidity and birefringence were measured by the optical detector. Residence time distribution curves (RTD) were obtained at various axial positions along three different kneading blocks and under a range of screw speeds. It is hypothesized that K, a parameter related to the area under each RTD curve, is a good indicator of dispersive mixing, whereas variance can be used to assess distributive mixing. The experimental data confirmed that these mixing indices are sensitive to changes in processing conditions, and that they translate the expected behavior of each kneading block geometry.

In-extruder measurements of shear viscosity and normal stresses are important as these measurement techniques allow determining the rheological state of the polymer melt at processing conditions up to high shear rates. However, validation of viscosity and normal stress data obtained by in-line slit rheometers at high shear rates is difficult due to a lack of overlap of the in-line data and the off-line measurements by rotational rheometers limited to lower shear rates. Here, shear viscosity and normal stress data measured in-line at large shear rates during extrusion and off-line at low shear rates are compared to predictions of the Doi-Edwards model and the Hierarchical Multi-Mode Molecular Stress Function (HMMSF) model using linear-viscoelastic off-line small amplitude oscillating shear data of two polystyrenes and a low-density polyethylene as input parameters. For polystyrene, the results of this investigation do not only validate the experimental data obtained by rotational as well as slit-die rheometry, but also demonstrate the agreement between experiments and models up to very high shear rates, which were not experimentally accessible earlier. The low-density polyethylene shows a more complex behaviour, which follows the HMMSF model at low shear rates, but approaches the Doi-Edwards model at high shear rates.