From Bottle Caps to Frisbee-A Case Study on Mechanical Recycling of Plastic Waste towards a Circular Economy.

This study demonstrates an open-loop recycling process of a specific post-consumer plastic waste stream. The targeted input waste material was defined as high-density polyethylene beverage bottle caps. Two methods of waste collection, informal and formal, were employed. Thereafter, materials were hand-sorted, shredded, regranulated, and then injection-molded into a flying disc (i.e., frisbee) as a pilot product. To observe the potential changes in the material throughout the entire recycling process, eight different test methods including melt mass-flow rate (MFR), differential scanning calorimetry (DSC), and mechanical tests were carried out on the various material states. The study showed that the informal collection led to a relatively higher purity in the input stream, which also appeared to have a 23% lower MFR value compared to that of the formally collected materials. The DSC measurements revealed a cross-contamination by polypropylene, which clearly affected the properties of all investigated materials. The cross-contamination led to a slightly higher tensile modulus in the recyclate, while the Charpy notched impact strength declined after processing by approximately 15% and 8% compared to those of the informal and formal input materials, respectively. All materials and the processing data were documented and stored online as a practical implementation of a digital product passport as a potential digital traceability tool. Furthermore, the suitability of the resulting recyclate to be used in transport packaging applications was also investigated. It was found that a direct replacement of virgin materials for this specific application is not possible without proper material modification.

Polypropylene Post-Consumer Recyclate Compounds for Thermoforming Packaging Applications.

Polypropylene (PP) plastic packaging waste consists of a variety of different plastic packaging products with a great span in rheological and mechanical behavior. Therefore, the resulting post-consumer recyclates usually show melt mass-flow rates (MFR) in the region of injection molding grades and intermediate mechanical properties. High-quality packaging applications demand a distinct property profile that is met by tailor-made PP grades and cannot be met by recyclates with intermediate performance. One such application with high market volume is high-stiffness thermoforming trays. The aim of this research was to blend intermediate-performance recyclates with a virgin PP grade to obtain compounds that fulfill the rheological and mechanical demands of this application. Three commercially available PP post-consumer recyclates were acquired and compounded with different blending ratios with a high stiffness, low MFR virgin PP grade. As the pure recyclates show different rheological properties, the blending ratios had to be adapted for each of them to fit into the MFR range of 2-4 g/10 min which is desirable for thermoforming applications. The resulting PP recyclate compounds show a distinct correlation of recyclate content with rheological and mechanical performance. However, the resulting property profile was directly dependent on the performance of the originally used recyclate. The best-performing recyclate could be used in a blending ratio of 65 m% recyclate content while adhering to both property limits, the MFR of 2-4 g/10 min and the lower bound tensile stiffness of 1500 MPa.

Polypropylene Pipe Compounds with Varying Post-Consumer Packaging Recyclate Content.

The high recycling targets set by the European Commission will create an increased availability of polypropylene (PP) post-consumer recyclates (PCRs). However, no regulations mandate the use of recycled PP (rPP), so the industry is challenged to explore possibilities to utilize such materials. One option, as suggested by the European Commission, is the introduction of rPP in pipe applications. According to existing standards, the use of recyclate is not allowed in pressurized gas and drinking water systems. However, many other pipe and underground applications, such as stormwater systems, open the increased use of PCRs. Additionally, even for less-demanding applications, such as non-pressure sewage systems, highly durable solutions are needed to cover the requested lifetime and request an ambitious property profile to fulfill the application needs that cannot be met by PP packaging materials and even less by PCRs thereof. Hence, this work explores the possible use of commercially available PCRs out of polypropylene from packaging applications in compounds together with virgin PP pipe grades to meet the demands for less-demanding applications. Two different commercially available rPPs and one commercially available recycled polyolefin (rPO) from mixed polyethylene and PP waste were acquired and, together with two predefined virgin PP pipe grades, were blended to compounds in the range of 10 m%, 20 m%, and 30 m% recyclate content. The compounds and three virgin PP pipe grades, acting as benchmarks, were tested in terms of short- and long-term mechanical performance as well as for many other physical properties. All of the compounds showed good results regarding fatigue crack (FCG) resistance with virgin polymer as the reference. The factors influencing FCG resistance, such as melt flow rate and polyolefin cross-contamination, were thoroughly investigated as the used virgin grades and recyclates cover a broad range of these properties.

Short- and Long-Term Performance of Pipe Compounds Containing Polyethylene Post-Consumer Recyclates from Packaging Waste.

The polymer industry is pushed to present solutions that lead to a circular plastics economy. High plastic packaging waste recycling targets will eventually lead to a high availability of packaging material recyclates. Although the use of polyethylene terephthalate (PET) recyclates is prescribed by regulations to be used in new PET bottles, no such regulation prescribes the use of polyethylene recyclate (rPE) in new products. One possibility of using rPE, which is considered by the European Union, is the use within pipe materials. Pipe applications demand a certain property profile, most prominently a high slow crack growth (SCG) resistance, which is not met by most packaging materials or recyclates made from it. Hence, this work investigates the use of commercially available post-consumer recyclates out of high-density polyethylene from packaging applications in compounds together with high SCG-resistant virgin PE pipe material with a PE100-RC specification. Two rPEs were acquired from German producers and blended to compounds consisting of 25 m%, 50 m% and 75 m% recyclate. These compounds, together with the pure recyclates and several virgin pipe materials acting as benchmarks were tested in terms of short- and long-term mechanical performance and with other basic characterization methods. Several compounds exceeded the performance of one tested virgin PE pipe material, an injection molding PE80 grade, in several categories. The content of recyclate needed to outperform this benchmark grade was mostly dependent on the resulting melt flow rate (MFR) of the compound and thus also of the MFR of the pure recyclate. Furthermore, different levels of polypropylene contaminations within the recyclates resulted in differently contaminated compounds. This is proved to influence the SCG resistance too, as compounds of similar MFRs but with different SCG resistances were found.

Assessment of Commercially Available Polyethylene Recyclates for Blow Molding Applications by a Novel Environmental Stress Cracking Method.

The transition to a circular economy has a major impact on waste management and the reuse of materials. New mandatory recycling targets for plastics will lead to a high availability of recyclates. For these recyclates, useful applications need to be found. One potential application for recyclates is blow molding bottles as packaging for non-food contents. This study investigates commercially available post-consumer high-density polyethylene recyclates together with virgin blow molding grades in terms of their short-term mechanical properties and environmental stress cracking resistance. While the short-term mechanical properties showed only slightly lower performance than the tested virgin grades, the overall environmental stress cracking failure times of the recyclates were much lower compared to virgin materials, even though the crack-growth kinetics could be similar. Although neither the tensile nor the notched impact strength results of the two polyethylene recyclates revealed large differences, the stress intensity-factor-dependent crack-growth rates of both materials were significantly different.

Characterization of Composition and Structure-Property Relationships of Commercial Post-Consumer Polyethylene and Polypropylene Recyclates.

The current efforts in moving closer towards a circular plastics economy puts massive pressure on recycled plastics, especially recycled polyethylene (rPE) and recycled polypropylene (rPP) to enter new markets. Their market penetration remained low so far, despite PE and PP constituting the largest share of plastic wastes. However, with the current imperative of more circularity comes a new focus on performance of recyclates. Hence, a detailed understanding of composition and structure-property relationships of post-consumer recyclates has to be developed. Five recycling companies from the Austrian and German markets were asked to supply their purest high-quality rPE and rPP grades. These were characterized by differential scanning calorimetry (DSC), thermo-gravimetric analysis (TGA), and Fourier-transform infrared (FTIR) spectroscopy, and micro-imaging. Technological characterization included density measurements, determination of the melt flow rate (MFR), and Charpy impact testing. All recyclates contained diverse contaminants and inclusions ranging from legacy fillers like calcium carbonate to polymeric contaminants like polyamides or polyolefin cross-contamination. The overall amount, size, and distribution of contaminants varied significantly among suppliers. Furthermore, first structure-property relationships for polyolefin recyclates that link inorganic content and polymeric purity with density and impact performance could be derived.

Global and Local Aging in Differently Stabilized Polypropylenes Exposed to Hot Chlorinated Water with and without Superimposed Mechanical-Environmental Loads.

The influence of chlorinated water on the global and local aging behavior of polypropylene (PP) was investigated for three differently stabilized PP grades consisting of the same PP base polymer. While one of the PP grades contained only a processing stabilizer (PP-S0), the other two were modified with a primary phenolic antioxidant (PP-S1) and a combination of a primary phenolic antioxidant and a hindered amine stabilizer (PP-S3). To study global aging effects, micro-sized specimens were pre-exposed to chlorinated water (5 mg/L free chlorine) at 60 °C for up to 750 h. Over the entire exposure period, significant material aging was detected by monitoring a continuous decrease in stabilizer content, oxidation induction temperature, mean molar mass, and mechanical strain at break. In terms of aging resistance and ultimate mechanical performance, PP-S1 was found to outperform the other two material formulations under these test conditions. Moreover, superimposed mechanical-environmental fatigue tests with cracked round bar specimens were carried out with the three PP grades in non-chlorinated (0 mg/L free chlorine) and chlorinated (5 mg/L free chlorine) water at 80 °C and 95 °C to study local crack tip aging effects. While the fatigue crack growth resistance substantially deteriorated for all three materials in chlorinated water, a significantly stronger effect was found for the higher temperature, with crack growth rates at a given stress intensity factor range in chlorinated water being ca. 30 to 50 times faster than in non-chlorinated water, depending on the material. Molar mass measurements of material samples taken from various positions of the tested CRB specimens provided clear evidence of enhanced local crack tip aging due to the chlorinated water environment.

Chlorinated Water Induced Aging of Pipe Grade Polypropylene Random Copolymers.

Polypropylene random copolymers (PP-R) are common materials for pressurized hot water pipes. In many pipe systems, potable water is disinfected by chlorine to prevent waterborne diseases. This paper deals with hot chlorinated water induced aging of two PP-R grades with varying morphology. One material had a conventional monoclinic α crystal form (PP-Rα), whereas the other was explicitly beta-nucleated resulting in a trigonal ß crystal form with a fine spherulite structure (PP-Rß). Micro-sized specimens with a thickness of 100 µm were used for aging experiments at 60 °C in chlorinated water with 5 mg/L free chlorine, and aging indicators were monitored for exposure times of up to 2000 h. On the other hand, superimposed mechanical-environmental tests were carried out by using cracked round bar specimens with a diameter of 14 mm to determine the fatigue crack growth (FCG) resistance of both PP-R grades at 60 °C in non-chlorinated and chlorinated water. PP-Rß was found to outperform PP-Rα with an about 30% higher time-to-embrittlement value of 2000 h. Furthermore, PP-Rß exhibited an enhanced FCG resistance in both non-chlorinated and chlorinated water. The effect of chlorine content on the deterioration of the FCG resistances was significantly more pronounced for PP-Rα.