Polylactide (PLA) is known as one of the most promising biopolymers as it is derived from renewable feedstock and can be biodegraded. During the last two decades, it moved more and more into the focus of scientific research and industrial use. It is even considered as a suitable replacement for standard petroleum-based polymers, such as polystyrene (PS), which can be found in a wide range of applications—amongst others in foams for packaging and insulation applications—but cause strong environmental issues. PLA has comparable mechanical properties to PS. However, the lack of melt strength is often referred to as a drawback for most foaming processes. One way to overcome this issue is the incorporation of chemical modifiers which can induce chain extension, branching, or cross-linking. As such, a wide variety of substances were studied in the literature. This work should give an overview of the most commonly used chemical modifiers and their effects on rheological, thermal, and foaming behavior. Therefore, this review article summarizes the research conducted on neat and chemically modified PLA foamed with the conventional foaming methods (i.e., batch foaming, foam extrusion, foam injection molding, and bead foaming).
Biodegradable plastics can make an important contribution to the struggle against increasing environmental pollution through plastics. However, biodegradability is a material property that is influenced by many factors. This review provides an overview of the main environmental conditions in which biodegradation takes place and then presents the degradability of numerous polymers. Polylactide (PLA), which is already available on an industrial scale, and the polyhydroxyalkanoates polyhydroxybutyrate (PHB) and polyhydroxybutyrate-co-valerate (PHBV), which are among the few plastics that have been proven to degrade in seawater, will be discussed in detail, followed by a summary of the degradability of further petroleum-, cellulose-, starch-, protein- and CO2-based biopolymers and some naturally occurring polymers.
The cyclic amide ε-caprolactam (ε-CLA) is efficiently polymerized by thermally latent C-2-protected N-heterocyclic carbenes (NHCs) to give the corresponding polyamide (PA 6). Carbon dioxideand metal salt-protected NHCs were used as precatalysts, out of which the free carbenes were generated thermally. This way, a premixing of the corresponding initiator with ε-CLA was possible to yield a storable and directly polymerizable mixture. The screening of a variety of differently constituted carbenes showed the importance of basicity of the active species, thereby revealing N-alkyl-bearing tetrahydropyrimidinium-based carbenes as the most active ones. Rapid production of PA 6 in high yields was possible in bulk polymerization at 180 °C, the best activity displayed by 1,3-dicyclohexyltetrahydropyrimidinium-2-carboxylate (6-Cy-CO 2 ). In situ rheology during polymerization showed the characteristics typical for the anionic polymerization of ε-CLA.
Laurolactam (LL) is polymerized in the bulk using strongly basic N-heterocyclic carbenes (NHCs) as initiators at temperatures of 180−200 °C to prepare the corresponding polyamide (PA 12). In-situ rheology of the polymerization progress reveals that an anionic mechanism is active, which is supported by the strong dependence of initiator activity on the basicity of the NHCs. GPC data and kinetic investigations show the process to be moderately controlled and fast, allowing high or quantitative yields in short polymerization times. Fifteen different NHC−CO 2 −adducts and NHC−metal complexes were used as thermally labile but room temperature stable NHC-precursors. Depending on the ring size and N-substituent, some of these protected NHCs allow forming a mixture of monomer and NHC-precursor that is suitable for long-term storage and readily polymerizable by simple heating. All polymerizations are executed without activator or other additives and thus represent a true one-component system for the production of PA 12. Finally, LL is copolymerized with εcaprolactam (ε-CLA). It is found that a copolymer with a considerable gradient is formed, with ε-CLA being incorporated preferentially at the onset of the polymerization.
Incorporation of agricultural wastes as fillers in fiber-reinforced plastics is gaining momentum in plastics engineering research. In this study, fiber-reinforced polypropylene (PP) with rice and coffee husks as filler material were developed. The effect of alkali (sodium hydroxide) pretreatment of the husks on mechanical and thermal properties of developed PP biocomposites was observed. Filler material loading was varied from 0% to 20% for rice husks and 0% to 10% for coffee husks. A twin-screw extruder was used for compounding the PP matrix with rice and coffee husk filler materials. Tensile strengths and percentage elongation results varied from 27.4 to 37.4 MPa and 2.4% to 70.3% (unmodified coffee husks), 31.1 to 37.4 MPa and 5% to 70.3% (unmodified rice husks), 30.7 to 37.4 MPa and 5.3% to 70.3% (modified coffee husks), and 30.7 to 37.4 MPa and 4.8% to 70.3% (modified rice husks). Young’s modulus ranged between 1656 and 2247.8 MPa for biocomposite PP samples with unmodified filler material. Young’s modulus ranged between 1740 and 2160 MPa after alkali treatment of the filler material. Charpy impact strengths ranged from 1.2 to 4 kJ/m2 and 3.1 to 19.6 kJ/m2 for samples containing unmodified and modified filler material, respectively. Thermogravimetric analysis showed that an increase in filler content resulted into delayed weight loss at high degradation temperatures. The results suggest that these developed fiber-reinforced plastics can be used in applications requiring high thermal stability and good mechanical properties.
Today PLA is one of the most important bioplastics on the market. A disadvantage of commercial polylactide is that it is not readily foamable, due to its low molecular weight, its low melt stability, and the lack of strain hardening effects. Therefore, commercially available polylactide has to be modified. In this study, the effects on properties by adding different modifiers were investigated. Adding of the modifiers and their chemical reaction were performed by means of reactive extrusion on a twin screw extruder. The molecular weight was increased by modifiers, which can be attributed to a changed chain topology. The highest molecular weight was achieved with organic peroxide. The rheological studies show that a changed chain topology can be assumed for the modified PLA. The most pronounced effect on the melt properties-the melt viscosity and also the melt strength-again was observed with the organic peroxide. The melt strength was increased for PLA modified with the organic peroxide. Furthermore, the organic peroxide was the only modifier that enhanced the crystallization rate, which is also favorable for extrusion foaming.
Biocomposites containing natural fibers and biopolymers are an ideal choice for developing substantially biodegradable materials for different applications. Polylactic acid is a biopolymer produced from renewable resources and has drawn numerous interest in packaging, electrical, and automotive application in recent years. However, its potential application in both electrical and automotive industries is limited by its flame retardancy and thermal properties. One way to offset this challenge has been to incorporate natural or synthetic flame retardants in polylactic acid (PLA). The aim of this article is to review the trends in research and development of composites based on agricultural fibers and PLA biopolymers over the past decade. This article highlights recent advances in the fields of flame retardancy and thermal stability of agricultural fiber‐reinforced PLA. Typical fiber‐reinforced PLA processing techniques are mentioned. Over 75% of the studies reported that incorporation of agricultural fibers resulted in enhanced flame retardancy and thermal stability of fiber‐reinforced PLA. These properties are further enhanced with surface modifications on the agricultural fibers prior to use as reinforcement in fiber‐reinforced PLA. From this review it is clear that flame retardancy and thermal stability depends on the type and pretreatment method of the agricultural fibers used in developing fiber‐reinforced PLA. Further research and development is encouraged on the enhancement of the flame retardancy properties of agricultural fiber‐reinforced PLA, especially using agricultural fibers themselves as flame retardants as opposed to synthetic flame retardants that are typically used.
Hydrogels are an interesting class of materials used in extrusion-based 3D printing, e.g., for drug delivery or tissue engineering. However, new hydrogel formulations for 3D printing as well as a detailed understanding of crucial formulation properties for 3D printing are needed. In this contribution, hydrogels based on poly(ethylene glycol) diacrylate (PEG-DA) and the charged monomers 3-sulfopropyl acrylate and [2-(acryloyloxy)ethyl]trimethylammonium chloride are formulated for 3D printing, together with Poloxamer 407 (P407). Chemical curing of formulations with PEG-DA and up to 5% (w/w) of the charged monomers was possible without difficulty. Through careful examination of the rheological properties of the non-cured formulations, it was found that flow properties of formulations with a high P407 concentration of 22.5% (w/w) possessed yield stresses well above 100 Pa together with pronounced shear thinning behavior. Thus, those formulations could be processed by 3D printing, as demonstrated by the generation of pyramidal objects. Modelling of the flow profile during 3D printing suggests that a plug-like laminar flow is prevalent inside the printer capillary. Under such circumstances, fast recovery of a high vicosity after material deposition might not be necessary to guarantee shape fidelity because the majority of the 3D printed volume does not face any relevant shear stress during printing.
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