Advanced Recycling of Plastic Waste: An Approach for Circular Economy

A special issue of Polymers (ISSN 2073-4360). This special issue belongs to the section "Circular and Green Polymer Science".

Deadline for manuscript submissions: closed (1 November 2023) | Viewed by 58268

Special Issue Editors

Research Institute for the Creation of Functional and Structural Materials, Fukuoka University, 8-19-1 Nanakuma, Jonan-ku, Fukuoka 814-0180, Japan
Interests: plastic mechanical recycling; polymer degradation; mechanical properties; recycling technology; structure–property relationship; polymer processing; surface modification; nanocellulose
Department of Chemical Engineering, Faculty of Engineering, Fukuoka University, Fukuoka, Japan
Interests: polymer physics; functional materials; mechanical recycling

Special Issue Information

Dear Colleagues,

Recycling is one approach to the reduction of plastic waste in the environment by reprocessing it into new products. Plastic recycling begins with the collection and separation of waste by type. This is followed by the recycling process, which consists of different approaches: mechanical recycling, chemical recycling, and energy recovery. However, all existing plastic recycling techniques are obstructed by limitations such as degradation of the mechanical properties of recycled products, the emission of volatile matters, and the high cost of operation. From these challenging points, the development of plastic recycling techniques is highly attractive for the promotion of circular economy and the sustainability of the environment.  

Dr. Patchiya Phanthong
Prof. Dr. Shigeru Yao
Guest Editors

Manuscript Submission Information

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Keywords

  • plastic circular economy
  • plastic recycling
  • polymer degradation
  • regeneration of plastic properties
  • plastic waste management
  • life cycle assessment
  • sustainability
  • design for advanced recycling technology
  • structure and properties of plastic
  • simulation of a new plastic recycling approach

Published Papers (27 papers)

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24 pages, 9841 KiB  
Article
Preparation and Characterization of High-Density Polyethylene with Alternating Lamellar Stems Using Molecular Dynamics Simulations
by Mohammed Althaf Hussain, Takashi Yamamoto, Syed Farooq Adil and Shigeru Yao
Polymers 2024, 16(2), 304; https://doi.org/10.3390/polym16020304 - 22 Jan 2024
Viewed by 661
Abstract
Mechanical recycling is the most efficient way to reduce plastic pollution due to its ability to maintain the intrinsic properties of plastics as well as provide economic benefits involved in other types of recycling. On the other hand, molecular dynamics (MD) simulations provide [...] Read more.
Mechanical recycling is the most efficient way to reduce plastic pollution due to its ability to maintain the intrinsic properties of plastics as well as provide economic benefits involved in other types of recycling. On the other hand, molecular dynamics (MD) simulations provide key insights into structural deformation, lamellar crystalline axis (c-axis) orientations, and reorganization, which are essential for understanding plastic behavior during structural deformations. To simulate the influence of structural deformations in high-density polyethylene (HDPE) during mechanical recycling while paying attention to obtaining an alternate lamellar orientation, the authors examine a specific way of preparing stacked lamella-oriented HDPE united atom (UA) models, starting from a single 1000 UA (C1000) chain of crystalline conformations and then packing such chain conformations into 2-chain, 10-chain, 15-chain, and 20-chain semi-crystalline models. The 2-chain, 10-chain, and 15-chain models yielded HDPE microstructures with the desired alternating lamellar orientations and entangled amorphous segments. On the other hand, the 20-chain model displayed multi-nucleus crystal growth instead of the lamellar-stack orientation. Structural characterization using a one-dimensional density profile and local order parameter {P2(r)} analyses demonstrated lamellar-stack orientation formation. All semi-crystalline models displayed the total density (ρ) and degree of crystallinity (χ) range of 0.90–0.94 g/cm−3 and ≥42–45%, respectively. A notable stress yield (σ_yield) ≈ 100–120 MPa and a superior elongation at break (ε_break) ~250% was observed under uniaxial strain deformation along the lamellar-stack orientation. Similarly, during the MD simulations, the microstructure phase change represented the average number of entanglements per chain (<Z>). From the present study, it can be recommended that the 10-chain alternate lamellar-stack orientation model is the most reliable miniature model for HDPE that can mimic industrially relevant plastic behavior in various conditions. Full article
(This article belongs to the Special Issue Advanced Recycling of Plastic Waste: An Approach for Circular Economy)
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18 pages, 6700 KiB  
Article
Feasibility Study for Finding Mathematical Approaches to Describe the Optimal Operation Point of Sensor-Based Sorting Machines for Plastic Waste
by Karl Friedrich, Nikolai Kuhn, Roland Pomberger and Gerald Koinig
Polymers 2023, 15(21), 4266; https://doi.org/10.3390/polym15214266 - 30 Oct 2023
Viewed by 713
Abstract
At present, sensor-based sorting machines are usually not operated at the optimal operation point but are either overrun or underrun depending on the availability of waste streams. Mathematical approaches for predefined ideal mixtures can be found based on the input stream composition and [...] Read more.
At present, sensor-based sorting machines are usually not operated at the optimal operation point but are either overrun or underrun depending on the availability of waste streams. Mathematical approaches for predefined ideal mixtures can be found based on the input stream composition and the throughput rate. This scientific article compares whether and under what conditions these approaches can be applied to sensor-based sorting machines. Existing data for predefined ideal mixtures are compared with newly generated data of real waste on three sensor-based sorting setups in order to make significant statements. Five samples of 3D plastics at regular intervals were taken in a processing plant for refuse-derived fuels. With the comparison of all these results, four hypotheses were validated, related to whether the same mathematical approaches can be transferred from ideal mixtures to real waste and whether they can be transferred to sensor-based sorting machines individually or depending on the construction type. The developed mathematical approaches are regression models for finding the optimal operation point to achieve a specific sensor-based sorting result in terms of purity and recovery. For a plant operator, the main benefit of the findings of this scientific article is that purity could be increased by 20% without substantially adapting the sorting plant. Full article
(This article belongs to the Special Issue Advanced Recycling of Plastic Waste: An Approach for Circular Economy)
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13 pages, 1996 KiB  
Article
Viability of Glycolysis for the Chemical Recycling of Highly Coloured and Multi-Layered Actual PET Wastes
by Asier Asueta, Sixto Arnaiz, Rafael Miguel-Fernández, Jon Leivar, Izotz Amundarain, Borja Aramburu, Jose Ignacio Gutiérrez-Ortiz and Rubén López-Fonseca
Polymers 2023, 15(20), 4196; https://doi.org/10.3390/polym15204196 - 23 Oct 2023
Cited by 1 | Viewed by 1188
Abstract
The chemical recycling of poly(ethylene terephthalate) –PET– fractions, derived from actual household packaging waste streams, using solvolysis, was investigated. This recycling strategy was applied after a previous on-line automatic identification, by near-infrared spectroscopy –NIR–, and a subsequent selective sorting of the different PET [...] Read more.
The chemical recycling of poly(ethylene terephthalate) –PET– fractions, derived from actual household packaging waste streams, using solvolysis, was investigated. This recycling strategy was applied after a previous on-line automatic identification, by near-infrared spectroscopy –NIR–, and a subsequent selective sorting of the different PET materials that were present in the packaging wastes. Using this technology, it was possible to classify fractions exclusively including PET, virtually avoiding the presence of both other plastics and materials, such as paper, cardboard and wood, that are present in the packaging wastes, as they were efficiently recognised and differentiated. The simple PET fractions, including clear and monolayered materials, were adequate to be recycled by mechanical means meanwhile the complex PET fractions, containing highly coloured and multi-layered materials, were suitable candidates to be recycled by chemical routes. The depolymerisation capacity of the catalytic glycolysis, when applied to those complex PET wastes, was studied by evaluating the effect of the process parameters on the resulting formation and recovery of the monomer bis(2-hydroxyethyl) terephthalate –BHET– and the achieved quality of this reaction product. Comparable and reasonable results, in terms of monomer yield and its characteristics, were obtained independently of the type of complex PET waste that was chemically recycled. Full article
(This article belongs to the Special Issue Advanced Recycling of Plastic Waste: An Approach for Circular Economy)
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23 pages, 10725 KiB  
Article
Thermoplastic Electromagnetic Shielding Materials from the Integral Recycling of Waste from Electronic Equipment
by Mihaela Aradoaei, Romeo C. Ciobanu, Cristina Schreiner, Andrei George Ursan, Elena Gabriela Hitruc and Magdalena Aflori
Polymers 2023, 15(19), 3859; https://doi.org/10.3390/polym15193859 - 22 Sep 2023
Cited by 1 | Viewed by 693
Abstract
The European Green Deal’s goals are anticipated to be fulfilled in large part thanks to the New Circular Economy Action Plan. It is believed that recycling materials will have a significant positive impact on the environment, particularly in terms of reducing greenhouse gas [...] Read more.
The European Green Deal’s goals are anticipated to be fulfilled in large part thanks to the New Circular Economy Action Plan. It is believed that recycling materials will have a significant positive impact on the environment, particularly in terms of reducing greenhouse gas emissions and the impacts this will have on preventing climate change. Due to the complexity of the issue and its significant practical ramifications, the activity of Waste Electrical and Electronic Equipment (WEEE) collection networks is a subject of interest for researchers and managers, in accordance with the principles that recent laws have addressed in a large number of industrialized countries. The goal of this paper is to characterize and obtain composite materials using an injection process with a matrix of LDPE, PP, and HDPE, with up to a 10% addition of nonmetallic powders from PCBs and electronic parts from an integrated process of WEEE recycling. The composites present relevant thermal, electrical, and mechanical properties. Such composite materials, due to their relevant dielectric properties, may be further tested for applications in electromagnetic shielding at frequencies above 1 kHz, or for electromagnetic interference/electromagnetic compatibility (EMI/EMC and ESD) applications at lower frequencies due to their superior dielectric loss factor values, associated with relevant behaviors around exploitation temperatures, mainly for the electric, electronic, or automotive industries. Full article
(This article belongs to the Special Issue Advanced Recycling of Plastic Waste: An Approach for Circular Economy)
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40 pages, 5763 KiB  
Article
Pyrolysis of Automotive Shredder Residue (ASR): Thermogravimetry, In-Situ Synchrotron IR and Gas-Phase IR of Polymeric Components
by Isha Kohli, Srikanth Chakravartula Srivatsa, Oisik Das, Sheila Devasahayam, R. K. Singh Raman and Sankar Bhattacharya
Polymers 2023, 15(17), 3650; https://doi.org/10.3390/polym15173650 - 04 Sep 2023
Cited by 1 | Viewed by 831
Abstract
This article reports the characterisation of pyrolysis of automotive shredder residue using in situ synchrotron IR, gas-phase IR, and thermal analyses to explore if the automotive shredder residue can be converted into value-added products. When heating to ~600 °C at different heating rates, [...] Read more.
This article reports the characterisation of pyrolysis of automotive shredder residue using in situ synchrotron IR, gas-phase IR, and thermal analyses to explore if the automotive shredder residue can be converted into value-added products. When heating to ~600 °C at different heating rates, thermal analyses suggested one- to two-stage pyrolysis. Transformations in the first stage, at lower temperatures, were attributed to the degradation of carbonyl, hydroxyl, or carboxyl functional stabilisers (aldehyde and ether impurities, additives, and stabilisers in the ASR). The second stage transformations, at higher temperatures, were attributed to the thermal degradation of the polymer char. Simultaneous thermal analyses and gas-phase IR spectroscopy confirmed the evolution of the gases (alkanes (CH4), CO2, and moisture). The synchrotron IR data have demonstrated that a high heating rate (such as 150 °C/min) results in an incomplete conversion of ASRs unless sufficient time is provided. The thermogravimetry data fit the linearised multistage kinetic model at different heating rates. The activation energy of reactions varied between 24.98 and 124.94 kJ/mol, indicating a surface-controlled reaction exhibiting high activation energy during the initial stages and a diffusion and mass transfer control showing lower activation energy at the final stages. The corresponding frequency factors were in the range of 3.34 × 1013–5.68 × 101 mg−1/min for different pyrolysis stages. The evolution of the functional groups decreased with an increase in the heating rate. Full article
(This article belongs to the Special Issue Advanced Recycling of Plastic Waste: An Approach for Circular Economy)
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13 pages, 3288 KiB  
Article
Synthesis and Application of ZSM-5 Catalyst Supported with Zinc and/or Nickel in the Conversion of Pyrolytic Gases from Recycled Polypropylene and Polystyrene Mixtures under Hydrogen Atmosphere
by Diego Barzallo, Rafael Lazo, Carlos Medina, Carlos Guashpa, Carla Tacuri and Paúl Palmay
Polymers 2023, 15(16), 3329; https://doi.org/10.3390/polym15163329 - 08 Aug 2023
Viewed by 1166
Abstract
Currently, catalytic pyrolysis has become a versatile and highly useful technology in the treatment of different plastic wastes. Thus, the development of selective catalysts to carry out cracking reactions and obtain a greater fraction of the desired products is essential. This study focuses [...] Read more.
Currently, catalytic pyrolysis has become a versatile and highly useful technology in the treatment of different plastic wastes. Thus, the development of selective catalysts to carry out cracking reactions and obtain a greater fraction of the desired products is essential. This study focuses on the synthesis of monometallic (Ni) and bimetallic (Ni-Zn) catalysts supported on ZSM-5 zeolite using an impregnation and co-impregnation method, respectively. The obtained catalysts were characterized by FTIR spectroscopy, N2 adsorption/desorption measurements, scanning electron microscopy (SEM) and energy dispersive X-Ray spectroscopy (EDS), temperature programmed NH3 desorption (TPD-NH3) and thermogravimetric analysis (TGA). In this way, a mixture of polystyrene and polypropylene recycled with a catalyst/plastic waste ratio of 1:500 was used for pyrolysis tests. The best results were obtained using the Ni-Zn/ZSM-5 catalyst, which included better impregnation, increased surface acidity, decreased dispersion and a shorter reaction time in the catalytic pyrolysis process. Under the optimized conditions, catalytic pyrolysis showed an excellent performance to generate hydrocarbons of greater industrial interest. Full article
(This article belongs to the Special Issue Advanced Recycling of Plastic Waste: An Approach for Circular Economy)
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19 pages, 5672 KiB  
Article
Prospects for Recyclable Multilayer Packaging: A Case Study
by Martina Seier, Vasiliki-Maria Archodoulaki, Thomas Koch, Bernadette Duscher and Markus Gahleitner
Polymers 2023, 15(13), 2966; https://doi.org/10.3390/polym15132966 - 06 Jul 2023
Viewed by 2357
Abstract
Food preservation is an essential application for polymers, particularly in packaging. Complex multilayer films, such as those used for modified atmosphere packaging (MAP), extend the shelf life of sensitive foods. These mostly contain various polymers to achieve the necessary combination of mechanic, optic, [...] Read more.
Food preservation is an essential application for polymers, particularly in packaging. Complex multilayer films, such as those used for modified atmosphere packaging (MAP), extend the shelf life of sensitive foods. These mostly contain various polymers to achieve the necessary combination of mechanic, optic, and barrier properties that limit their recyclability. As the European Union’s Circular Economy Action Plan calls for sustainable products and business models, including waste prevention policies and recycling quotas, with plastic packaging being a high priority, solutions towards more sustainable multilayer packaging are urgently needed. This study evaluated and compared the recycling potential of functionally equivalent PET (polyethylene terephthalate) and PP (polypropylene) post-consumer MAP through structure analysis and recycling simulation. The structure analysis revealed that both types of MAP contained functional (stability) and barrier layers (oxygen and moisture). The recycling simulation showed that the PP-based packaging was recyclable 10 times, maintaining its mechanical properties and functionality. At the same time, the PET-based MAP resulted in a highly brittle material that was unsuitable for reprocessing into similar economic value products. The secondary material from the PP-based MAP was successfully manufactured into films, demonstrating the functional possibility of closed-loop recycling. The transition from a linear to a circular economy for MAP is currently still limited by safety concerns due to a lack of sufficient and efficient purification methods, but the proper design of multilayers for recyclability is a first step towards circularity. Full article
(This article belongs to the Special Issue Advanced Recycling of Plastic Waste: An Approach for Circular Economy)
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17 pages, 4946 KiB  
Article
The Development of Environmentally Sustainable Poly(vinyl chloride) Composite from Waste Non-Metallic Printed Circuit Board with Interfacial Agents
by Aung Kyaw Moe, Jirasuta Chungprempree, Jitima Preechawong, Pornsri Sapsrithong and Manit Nithitanakul
Polymers 2023, 15(13), 2938; https://doi.org/10.3390/polym15132938 - 04 Jul 2023
Cited by 2 | Viewed by 1428
Abstract
The recycling of non-metallic printed circuit boards (NMPCB) as a filler in poly(vinyl chloride) (PVC) composite would help to encourage the use of waste NMPCB, thus, reducing some environmental concerns with regard to e-waste. The objective of this study was to comprehensively evaluate [...] Read more.
The recycling of non-metallic printed circuit boards (NMPCB) as a filler in poly(vinyl chloride) (PVC) composite would help to encourage the use of waste NMPCB, thus, reducing some environmental concerns with regard to e-waste. The objective of this study was to comprehensively evaluate the effect of different interfacial agents, namely polypropylene grafted maleic anhydride (PP-g-MAH) and ϒ-aminopropyltriethoxy silane (ATPS) on the morphology and properties of PVC/NMPCB composites. A PVC/NMPCB composite was prepared by melt compounding with varying amounts of NMPCB ranging between 10, 20 and 30 wt.%. Fourier transform infrared spectroscopy–attenuated total reflectance (FTIR–ATR) analysis revealed the interactions between PVC and NMPCB when using both PP-g-MAH and ATPS interfacial agent. The properties and morphology of PVC/NMPCB composites were significantly dependent on the interfacial agent treated on the NMPCB surface. The phase morphology and mechanical properties of PVC/NMPCB composites (30 wt.% of NMPCB) were improved and the result also indicated that the higher compatibility of composites with ATPS as an interfacial agent led to our obtaining the maximum Young’s modulus of 484 MPa. The dynamic mechanical analysis revealed the interaction at the interface, with the Tg shifting to a lower temperature in the presence of PP-g-MAH and strong interfacial adhesion noted with the improved Tg in the presence of the ATPS interfacial agent. Further evidence of the improved interaction was observed with the increment in density in the presence of ATPS when compared with PP-g-MAH in PVC/NMPCB composite. Hence, of the two interfacial agents, ATPS showed itself to be more effective when employed as an interfacial agent for NMPCB in PVC composite for industry. Full article
(This article belongs to the Special Issue Advanced Recycling of Plastic Waste: An Approach for Circular Economy)
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24 pages, 8402 KiB  
Article
Chemical Recycling of Fully Recyclable Bio-Epoxy Matrices and Reuse Strategies: A Cradle-to-Cradle Approach
by Lorena Saitta, Giuliana Rizzo, Claudio Tosto, Gianluca Cicala, Ignazio Blanco, Eugenio Pergolizzi, Romeo Ciobanu and Giuseppe Recca
Polymers 2023, 15(13), 2809; https://doi.org/10.3390/polym15132809 - 25 Jun 2023
Cited by 1 | Viewed by 1382
Abstract
Currently, the epoxy resin market is expressing concerns about epoxy resins’ non-recyclability, which can hinder their widespread use. Moreover, epoxy monomers are synthesized via petroleum-based raw materials, which also limits their use. So, it is crucial to find more environmentally friendly alternative solution [...] Read more.
Currently, the epoxy resin market is expressing concerns about epoxy resins’ non-recyclability, which can hinder their widespread use. Moreover, epoxy monomers are synthesized via petroleum-based raw materials, which also limits their use. So, it is crucial to find more environmentally friendly alternative solution for their formulation. Within this context, the aim of this paper is to exploit a Cradle-to-Cradle approach, which consists of remodeling and reshaping the productive cycle of consumer products to make sure that they can be infinitely reused rather than just being recycled with a downgrading of their properties or uses, according to the principle of the complete circular economy. Indeed, after starting with a fully-recyclable bio-based epoxy formulation and assessing its recyclability as having a process yield of 99%, we obtained a recycled polymer that could be reused, mixing with the same bio-based epoxy formulation with percentages varying from 15 wt% to 27 wt%. The formulation obtained was thoroughly characterized by a dynamic-mechanical analysis, differential scanning calorimetry, and flexural tests. This approach had two advantages: (1) it represented a sustainable disposal route for the epoxy resin, with nearly all the epoxy resin recovered, and (2) the obtained recycled polymer could be used as a green component of the primary bio-based epoxy matrix. In the end, by using replicated general factorial designs (as statistical tools) combined with a proper optimization process, after carrying out a complete thermo-mechanical characterization of the developed epoxy formulations, the right percentage of recycled polymer content was selected with the aim of identifying the most performing epoxy matrix formulation in terms of its thermo-mechanical properties. Full article
(This article belongs to the Special Issue Advanced Recycling of Plastic Waste: An Approach for Circular Economy)
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15 pages, 4945 KiB  
Article
Understanding the Effect of Side Reactions on the Recyclability of Furan–Maleimide Resins Based on Thermoreversible Diels–Alder Network
by Brandon T. McReynolds, Kavon D. Mojtabai, Nicole Penners, Gaeun Kim, Samantha Lindholm, Youngmin Lee, John D. McCoy and Sanchari Chowdhury
Polymers 2023, 15(5), 1106; https://doi.org/10.3390/polym15051106 - 23 Feb 2023
Cited by 3 | Viewed by 2508
Abstract
We studied the effect of side reactions on the reversibility of epoxy with thermoreversible Diels–Alder (DA) cycloadducts based on furan and maleimide chemistry. The most common side reaction is the maleimide homopolymerization which introduces irreversible crosslinking in the network adversely affecting the recyclability. [...] Read more.
We studied the effect of side reactions on the reversibility of epoxy with thermoreversible Diels–Alder (DA) cycloadducts based on furan and maleimide chemistry. The most common side reaction is the maleimide homopolymerization which introduces irreversible crosslinking in the network adversely affecting the recyclability. The main challenge is that the temperatures at which maleimide homopolymerization can occur are approximately the same as the temperatures at which retro-DA (rDA) reactions depolymerize the networks. Here we conducted detailed studies on three different strategies to minimize the effect of the side reaction. First, we controlled the ratio of maleimide to furan to reduce the concentration of maleimide groups which diminishes the effects of the side reaction. Second, we applied a radical-reaction inhibitor. Inclusion of hydroquinone, a known free radical scavenger, is found to retard the onset of the side reaction both in the temperature sweep and isothermal measurements. Finally, we employed a new trismaleimide precursor that has a lower maleimide concentration and reduces the rate of the side reaction. Our results provide insights into how to minimize formation of irreversible crosslinking by side reactions in reversible DA materials using maleimides, which is important for their application as novel self-healing, recyclable, and 3D-printable materials. Full article
(This article belongs to the Special Issue Advanced Recycling of Plastic Waste: An Approach for Circular Economy)
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10 pages, 862 KiB  
Article
Can Pyrolysis Oil Be Used as a Feedstock to Close the Gap in the Circular Economy of Polyolefins?
by Berrak Erkmen, Adem Ozdogan, Ayhan Ezdesir and Gokhan Celik
Polymers 2023, 15(4), 859; https://doi.org/10.3390/polym15040859 - 09 Feb 2023
Cited by 2 | Viewed by 3861
Abstract
Plastics are engineering marvels that have found widespread use in all aspects of modern life. However, poor waste management practices and inefficient recycling technologies, along with their extremely high durability, have caused one of the major environmental problems facing humankind: waste plastic pollution. [...] Read more.
Plastics are engineering marvels that have found widespread use in all aspects of modern life. However, poor waste management practices and inefficient recycling technologies, along with their extremely high durability, have caused one of the major environmental problems facing humankind: waste plastic pollution. The upcycling of waste plastics to chemical feedstock to produce virgin plastics has emerged as a viable option to mitigate the adverse effects of plastic pollution and close the gap in the circular economy of plastics. Pyrolysis is considered a chemical recycling technology to upcycle waste plastics. Yet, whether pyrolysis as a stand-alone technology can achieve true circularity or not requires further investigation. In this study, we analyzed and critically evaluated whether oil obtained from the non-catalytic pyrolysis of virgin polypropylene (PP) can be used as a feedstock for naphtha crackers to produce olefins, and subsequently polyolefins, without undermining the circular economy and resource efficiency. Two different pyrolysis oils were obtained from a pyrolysis plant and compared with light and heavy naphtha by a combination of physical and chromatographic methods, in accordance with established standards. The results demonstrate that pyrolysis oil consists of mostly cyclic olefins with a bromine number of 85 to 304, whereas light naphtha consists of mostly paraffinic hydrocarbons with a very low olefinic content and a bromine number around 1. Owing to the compositional differences, pyrolysis oil studied herein is completely different than naphtha in terms of hydrocarbon composition and cannot be used as a feedstock for commercial naphtha crackers to produce olefins. The findings are of particular importance to evaluating different chemical recycling opportunities with respect to true circularity and may serve as a benchmark to determine whether liquids obtained from different polyolefin recycling technologies are compatible with existing industrial steam crackers’ feedstock. Full article
(This article belongs to the Special Issue Advanced Recycling of Plastic Waste: An Approach for Circular Economy)
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15 pages, 1945 KiB  
Article
Removal of Bromine from Polymer Blends with a Composition Simulating That Found in Waste Electric and Electronic Equipment through a Facile and Environmentally Friendly Method
by Maria Anna Charitopoulou, Lambrini Papadopoulou and Dimitris S. Achilias
Polymers 2023, 15(3), 709; https://doi.org/10.3390/polym15030709 - 31 Jan 2023
Cited by 1 | Viewed by 1523
Abstract
The increasing volume of plastics from waste electric and electronic equipment (WEEE) nowadays is of major concern since the various toxic compounds that are formed during their handling enhance the difficulties in recycling them. To overcome these problems, this work examines solvent extraction [...] Read more.
The increasing volume of plastics from waste electric and electronic equipment (WEEE) nowadays is of major concern since the various toxic compounds that are formed during their handling enhance the difficulties in recycling them. To overcome these problems, this work examines solvent extraction as a pretreatment method, prior to thermochemical recycling by pyrolysis. The aim is to remove bromine from some polymeric blends, with a composition that simulates WEEE, in the presence of tetrabromobisphenol A (TBBPA). Various solvents—isopropanol, ethanol and butanol—as well as several extraction times, were investigated in order to find the optimal choice. Before and after the pretreatment, blends were analysed by X-ray fluorescence (XRF) to estimate the total bromine content. Blends were pyrolyzed before and after the soxhlet extraction in order to evaluate the derived products. FTIR measurements of the polymeric blends before and after the soxhlet extraction showed that their structure was maintained. From the results obtained, it was indicated that the reduction of bromine was achieved in all cases tested and it was ~34% for blend I and ~46% and 42% for blend II when applying a 6 h soxhlet with isopropanol and ethanol, respectively. When using butanol bromine was completely eliminated, since the reduction reached almost 100%. The latter finding is of great importance, since the complete removal of bromine enables the recycling of pure plastics. Therefore, the main contribution of this work to the advancement of knowledge lies in the use of a solvent (i.e., butanol) which is environmentally friendly and with a high dissolving capacity in brominated compounds, which can be used in a pretreatment stage of plastic wastes before it is recycled by pyrolysis. Full article
(This article belongs to the Special Issue Advanced Recycling of Plastic Waste: An Approach for Circular Economy)
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19 pages, 5428 KiB  
Article
Polypropylene Pipe Compounds with Varying Post-Consumer Packaging Recyclate Content
by Paul J. Freudenthaler, Joerg Fischer, Yi Liu and Reinhold W. Lang
Polymers 2022, 14(23), 5232; https://doi.org/10.3390/polym14235232 - 01 Dec 2022
Cited by 4 | Viewed by 1319
Abstract
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 [...] Read more.
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. Full article
(This article belongs to the Special Issue Advanced Recycling of Plastic Waste: An Approach for Circular Economy)
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18 pages, 2096 KiB  
Article
Selection of Conditions in PVB Polymer Dissolution Process for Laminated Glass Recycling Applications
by Marek Królikowski, Piotr Żach and Maciej Kalestyński
Polymers 2022, 14(23), 5119; https://doi.org/10.3390/polym14235119 - 24 Nov 2022
Viewed by 1926
Abstract
Polyvinyl(butyral) (PVB) post-production waste collected from the windshields of end-of-life vehicles and post-consumer building laminated glass are valuable polymeric materials that can be reused. Every year, large amounts of PVB waste are still being buried in landfills owing to a lack of appropriate [...] Read more.
Polyvinyl(butyral) (PVB) post-production waste collected from the windshields of end-of-life vehicles and post-consumer building laminated glass are valuable polymeric materials that can be reused. Every year, large amounts of PVB waste are still being buried in landfills owing to a lack of appropriate recycling techniques. Before reuse, PVB should be thoroughly cleaned of solid contaminants such as glass dust, fused heating wires, and other waste polymers, metals, and ceramics. This can be done by polymer dissolution and filtration. In this study, we propose the purification of PVB from contamination by dissolving the post-consumer polymeric materials into single and binary organic solvents. As part of the experimental work, measurements and optimization of the dissolution time of PVB were performed. PVB dissolves faster when a binary solvent (2-propanol + ethyl acetate) than pure 2-propanol is used. From the point of view of the practical application of PVB solutions, measurements of density and dynamic viscosity as a function of PVB concentration and temperature were performed. The PVB solutions obtained in this work can be widely used as glues for glass, ceramics, metal, impregnating, and insulating materials or as paint additives that are entirely transparent for visible light and to block UV rays. Full article
(This article belongs to the Special Issue Advanced Recycling of Plastic Waste: An Approach for Circular Economy)
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18 pages, 2392 KiB  
Article
The Effect of Various Polyhedral Oligomeric Silsesquioxanes on Viscoelastic, Thermal Properties and Crystallization of Poly(ε-caprolactone) Nanocomposites
by Magdalena Lipińska
Polymers 2022, 14(23), 5078; https://doi.org/10.3390/polym14235078 - 23 Nov 2022
Cited by 3 | Viewed by 1039
Abstract
Polyhedral oligomeric silsesquioxane POSS nanoparticles can be applied as reinforcing additives modifying various properties of biodegradable polymers. The effects of aminopropylisobutyl POSS (amine-POSS), trisilanolisooctyl-POSS (HO-POSS) and glycidyl-POSS (Gly-POSS) on the viscoelastic, thermal properties and crystallization of biodegradable poly(ε-caprolactone) PCL were studied. The analysis [...] Read more.
Polyhedral oligomeric silsesquioxane POSS nanoparticles can be applied as reinforcing additives modifying various properties of biodegradable polymers. The effects of aminopropylisobutyl POSS (amine-POSS), trisilanolisooctyl-POSS (HO-POSS) and glycidyl-POSS (Gly-POSS) on the viscoelastic, thermal properties and crystallization of biodegradable poly(ε-caprolactone) PCL were studied. The analysis of the viscoelastic properties at ambient temperature indicated that aminopropylisobutyl POSS (amine-POSS) and glycidyl-POSS (Gly-POSS) enhanced the dynamic mechanical properties of PCL. The increase in the storage shear modulus G′ and loss modulus G″ was observed. The plasticizing effect of trisilanolisooctyl POSS (HO-POSS) due to the presence of long isoctyl groups was confirmed. As a result, the crystallization of PCL was facilitated and the degree of crystallinity of χc increased up to 50.9%. The damping properties and the values of tan δ for PCL/HO-POSS composition increased from 0.052 to 0.069. The TGA results point out the worsening of the PCL thermal stability, with lower values of T0.5%, T1% and T3%. Both HO-POSS and Gly-POSS facilitated the relaxation of molten PCL. The presence of Gly-POSS influenced the changes that occurred in the viscoelastic properties of the molten PCL due to the thermo-mechanical degradation of the material; a positive impact was observed. Full article
(This article belongs to the Special Issue Advanced Recycling of Plastic Waste: An Approach for Circular Economy)
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17 pages, 3630 KiB  
Article
Effects of Heating Rate and Temperature on the Thermal Pyrolysis of Expanded Polystyrene Post-Industrial Waste
by Arantxa M. Gonzalez-Aguilar, Victoria P. Cabrera-Madera, James R. Vera-Rozo and José M. Riesco-Ávila
Polymers 2022, 14(22), 4957; https://doi.org/10.3390/polym14224957 - 16 Nov 2022
Cited by 6 | Viewed by 2619
Abstract
The use of plastic as material in various applications has been essential in the evolution of the technology industry and human society since 1950. Therefore, their production and waste generation are high due to population growth. Pyrolysis is an effective recycling method for [...] Read more.
The use of plastic as material in various applications has been essential in the evolution of the technology industry and human society since 1950. Therefore, their production and waste generation are high due to population growth. Pyrolysis is an effective recycling method for treating plastic waste because it can recover valuable products for the chemical and petrochemical industry. This work addresses the thermal pyrolysis of expanded polystyrene (EPS) post-industrial waste in a semi-batch reactor. The influence of reaction temperature (350–500 °C) and heating rate (4–40 °C min−1) on the liquid conversion yields and physicochemical properties was studied based on a multilevel factorial statistical analysis. In addition, the analysis of the obtaining of mono-aromatics such as styrene, toluene, benzene, ethylbenzene, and α-methyl styrene was performed. Hydrocarbon liquid yields of 76.5–93% were achieved at reaction temperatures between 350 and 450 °C, respectively. Styrene yields reached up to 72% at 450 °C and a heating rate of 25 °C min−1. Finally, the potential application of the products obtained is discussed by proposing the minimization of EPS waste via pyrolysis. Full article
(This article belongs to the Special Issue Advanced Recycling of Plastic Waste: An Approach for Circular Economy)
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22 pages, 6102 KiB  
Article
Integrated Approach to Eco-Friendly Thermoplastic Composites Based on Chemically Recycled PET Co-Polymers Reinforced with Treated Banana Fibres
by Martial Aime Kuete, Pascal Van Velthem, Wael Ballout, Bernard Nysten, Jacques Devaux, Maurice Kor Ndikontar, Thomas Pardoen and Christian Bailly
Polymers 2022, 14(22), 4791; https://doi.org/10.3390/polym14224791 - 08 Nov 2022
Cited by 4 | Viewed by 1643
Abstract
A major societal issue of disposal and environmental pollution is raised by the enormous and fast-growing production of single-use polyethylene terephthalate (PET) bottles, especially in developing countries. To contribute to the problem solution, an original route to recycle PET in the form of [...] Read more.
A major societal issue of disposal and environmental pollution is raised by the enormous and fast-growing production of single-use polyethylene terephthalate (PET) bottles, especially in developing countries. To contribute to the problem solution, an original route to recycle PET in the form of value-added environmentally friendly thermoplastic composites with banana fibres (Musa acuminata) has been developed at the laboratory scale. Banana fibres are a so far undervalued by-product of banana crops with great potential as polymer reinforcement. The melt-processing constraints of commercial PET, including used bottles, being incompatible with the thermal stability limits use of natural fibres; PET has been modified with bio-sourced reactants to produce co-polymers with moderate processing temperatures below 200 °C. First, commercial PET were partially glycolyzed with 1.3-propanediol to produce co-oligomers of about 20 repeating units, which were next chain extended with succinic anhydride and post-treated in a very unusual “soft solid state” process at temperatures in the vicinity of the melting point to generate co-polymers with excellent ductility. The molar mass build-up reaction is dominated by esterification of the chain ends and benefits from the addition of succinic anhydride to rebalance the acid-to-hydroxyl end-group ratio. Infra-red spectroscopy and intrinsic viscosity were extensively used to quantify the concentration of chain ends and the average molar mass of the co-polymers at all stages of the process. The best co-polymers are crystallisable, though at slow kinetics, with a Tg of 48 °C and a melting point strongly dependent upon thermal history. The composites show high stiffness (4.8 GPa at 20% fibres), consistent with the excellent dispersion of the fibres and a very high interfacial cohesion. The strong adhesion can be tentatively explained by covalent bonding involving unreacted succinic anhydride in excess during solid stating. A first approach to quantify the sustainable benefits of this PET recycling route, based on a rational eco-selection method, gives promising results since the composites come close to low-end wood materials in terms of the stiffness/embodied energy balance. Moreover, this approach can easily be extended to many other natural fibres. The present study is limited to a proof of concept at the laboratory scale but is encouraging enough to warrant a follow-up study toward scale-up and application development. Full article
(This article belongs to the Special Issue Advanced Recycling of Plastic Waste: An Approach for Circular Economy)
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17 pages, 4045 KiB  
Article
Recycling Waste Nonmetallic Printed Circuit Boards for Polyvinyl Chloride Composites
by Aung Kyaw Moe, Jirasuta Chungprempree, Jitima Preechawong, Pornsri Sapsrithong and Manit Nithitanakul
Polymers 2022, 14(17), 3531; https://doi.org/10.3390/polym14173531 - 28 Aug 2022
Cited by 6 | Viewed by 1703
Abstract
To reduce environmental threats, such as land filling, incineration and soil pollution, which are associated with the improper waste management of waste printed circuit boards, the utilization of NMPCBs from waste PCBs as a filler in composites was pursued. Untreated and treated NMPCBs [...] Read more.
To reduce environmental threats, such as land filling, incineration and soil pollution, which are associated with the improper waste management of waste printed circuit boards, the utilization of NMPCBs from waste PCBs as a filler in composites was pursued. Untreated and treated NMPCBs in varying ratios, 10–30 wt.%, were blended with PVC to produce NMPCB/PVC composites, using the melt-mixing method via an internal mixer, in order to solve the remaining NMPCB waste problem after the valuable metals in PCBs were recovered. The incorporation of the NMPCB with PVC resulted in an increase in the tensile modulus and the thermal stability of the resulting composites. Scanning electron microscopy (SEM) results indicated improved interfacial adhesion between the treated NMPCB and the PVC matrix. The FTIR results of the NMPCB treated with 3-glycidyloxypropyltrimethoxysilane (GPTMS) revealed the formation of Si-O-Si bonds. The densities of the composites were found to increase with an increase in the content of the treated NMPCB, and compatibility improved. The tensile properties of the treated NMPCB/PVC composites were higher than those of the untreated NMPCB/PVC composites, suggesting improved compatibility between the treated NMPCB and PVC. The PVC composite with 10 wt.% of the treated NMPCB showed the optimum tensile properties. It was observed that the tensile modulus of the treated NMPCB/PVC composite increased by 47.65% when compared to that of the neat PVC. The maximum thermal degradation temperature was 27 °C higher than that of the neat PVC. Dynamic mechanical analysis results also support the improved interfacial adhesion as a result of the improvement in the storage modulus at the glassy region, and the loss factor (tan δ) peak shifted to a higher temperature range than that of the PVC and the untreated NMPCB/PVC composite. These studies reveal that the NMPCB was successfully modified with 1 wt.% of GPTMS, which promoted the dispersion and interfacial adhesion in the PVC matrix, resulting in better tensile properties and better thermal stability of the PVC composite. Full article
(This article belongs to the Special Issue Advanced Recycling of Plastic Waste: An Approach for Circular Economy)
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13 pages, 4882 KiB  
Article
Verification of the Influence of Processing History through Comparing High-Speed Melt Spinning Behavior of Virgin and Recycled Polypropylene
by Wataru Takarada, Mohammad A. Barique, Tatsuma Kunimitsu, Takao Kameda and Takeshi Kikutani
Polymers 2022, 14(16), 3238; https://doi.org/10.3390/polym14163238 - 09 Aug 2022
Cited by 1 | Viewed by 1278
Abstract
A ‘model’ material of recycled polypropylene (PP) was prepared through the injection molding process, and the effect of processing history on the polymer characteristics was investigated through the high-speed melt spinning of virgin and recycled PP. On-line measurement of the thinning behavior of [...] Read more.
A ‘model’ material of recycled polypropylene (PP) was prepared through the injection molding process, and the effect of processing history on the polymer characteristics was investigated through the high-speed melt spinning of virgin and recycled PP. On-line measurement of the thinning behavior of the spin-line revealed the downstream shift of solidification point for the recycled PP at the take-up velocity of 1.0 km/min, indicating the suppression of flow-induced crystallization. The difference was not clear at higher take-up velocities of up to 5 km/min. For any identical take-up velocity, no clear difference in the stress-strain curves and birefringence of the fibers from virgin and recycled PP could be observed, whereas the detailed investigation on the variation of relative amount of c-axis and a*-axis oriented crystals in the fibers prepared at varied take-up velocities suggested the deterioration of flow-induced crystallization at 1.0 km/min. It was speculated that the processing history induced the lowering of the entanglement density, which affected the melt spinning and crystallization behavior. An undistinguishable difference between the virgin and recycled PP at increased take-up velocities suggested the existence of an optimum elongational strain rate for the detection of the different states of molecular entanglement. Full article
(This article belongs to the Special Issue Advanced Recycling of Plastic Waste: An Approach for Circular Economy)
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17 pages, 7502 KiB  
Article
Material Property Recovery by Controlling the Melt Memory Effects on Recrystallization and on Crystal Deformation: An Approach by the Molecular Dynamics Simulation for Polyethylene
by Takashi Yamamoto, Mohammed Althaf Hussain and Shigeru Yao
Polymers 2022, 14(15), 3082; https://doi.org/10.3390/polym14153082 - 29 Jul 2022
Cited by 1 | Viewed by 1654
Abstract
Degradation in the mechanical properties of recycled polymer materials has been recently appearing as a big issue in polymer science. The molecular mechanism of the degradation is considered in part due to residual memories of flow experienced during molding processes, and therefore the [...] Read more.
Degradation in the mechanical properties of recycled polymer materials has been recently appearing as a big issue in polymer science. The molecular mechanism of the degradation is considered in part due to residual memories of flow experienced during molding processes, and therefore the mechanical recycling through remolding involving melting and recrystallization has been attempted in recent years. In the present paper, the molecular processes of melting and recrystallization are investigated by the molecular dynamics simulation for polyethylene with special interest in the melt memory effects. We also studied the mechanical properties of the recrystalized materials that have undergone different recrystallization processes aiming to discover better recycling strategies. A successive step-by-step approach is adopted to study the loss of the crystal memory during retention in the melt, the effects of the melt memory on the mode of recrystallization, the relation between the recrystallization mode and the resulting higher-order structure, and the mechanical properties controlled by the higher-order structures. It is shown that the melt memory clearly remains in various order parameters that persist over time scales corresponding to the Rouse time, the remaining melt memory markedly affects the crystallization mode leading to distinct crystalline morphologies, and the distinct morphologies obtained give different mechanical responses during large deformations. Full article
(This article belongs to the Special Issue Advanced Recycling of Plastic Waste: An Approach for Circular Economy)
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17 pages, 2707 KiB  
Article
Bioconversion Process of Polyethylene from Waste Tetra Pak® Packaging to Polyhydroxyalkanoates
by Itohowo Ekere, Brian Johnston, Fideline Tchuenbou-Magaia, David Townrow, Szymon Wojciechowski, Adam Marek, Jan Zawadiak, Khadar Duale, Magdalena Zieba, Wanda Sikorska, Grazyna Adamus, Tomasz Goslar, Marek Kowalczuk and Iza Radecka
Polymers 2022, 14(14), 2840; https://doi.org/10.3390/polym14142840 - 12 Jul 2022
Cited by 9 | Viewed by 3881
Abstract
Presented herein are the results of a novel recycling method for waste Tetra Pak® packaging materials. The polyethylene (PE-T) component of this packaging material, obtained via a separation process using a “solvents method”, was used as a carbon source for the biosynthesis [...] Read more.
Presented herein are the results of a novel recycling method for waste Tetra Pak® packaging materials. The polyethylene (PE-T) component of this packaging material, obtained via a separation process using a “solvents method”, was used as a carbon source for the biosynthesis of polyhydroxyalkanoates (PHAs) by the bacterial strain Cupriavidus necator H16. Bacteria were grown for 48–72 h, at 30 °C, in TSB (nitrogen-rich) or BSM (nitrogen-limited) media supplemented with PE-T. Growth was monitored by viable counting. It was demonstrated that C. necator utilised PE-T in both growth media, but was only able to accumulate 40% w/w PHA in TSB supplemented with PE-T. Only 1.5% w/w PHA was accumulated in the TSB control, and no PHA was detected in the BSM control. Extracted biopolymers were characterised by nuclear magnetic resonance (NMR), Fourier-transform infrared (FTIR) spectroscopy, electrospray tandem mass spectrometry (ESI-MS/MS), gel permeation chromatography (GPC), and accelerator mass spectrometry (AMS). The characterisation of PHA by ESI-MS/MS revealed that PHA produced by C. necator in TSB supplemented with PE-T contained 3-hydroxybutyrate, 3-hydroxyvalerate, and 3-hydroxyhexanoate co-monomeric units. AMS analysis also confirmed the presence of 96.73% modern carbon and 3.27% old carbon in PHA derived from Tetra Pak®. Thus, this study demonstrates the feasibility of our proposed recycling method for waste Tetra Pak® packaging materials, alongside its potential for producing value-added PHA, and the ability of 14C analysis in validating this bioconversion process. Full article
(This article belongs to the Special Issue Advanced Recycling of Plastic Waste: An Approach for Circular Economy)
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13 pages, 2597 KiB  
Article
The Impact of Reprocessing with a Quad Screw Extruder on the Degradation of Polypropylene
by Mansour Alotaibi, Thamer Aldhafeeri and Carol Barry
Polymers 2022, 14(13), 2661; https://doi.org/10.3390/polym14132661 - 29 Jun 2022
Cited by 4 | Viewed by 2066
Abstract
During mechanical recycling, polypropylene typically is reprocessed using a single- or twin-screw extruder. The degradation of polypropylene during this reprocessing reduces the polymer’s molecular weight and, consequently, limits the performance of the recycled resin. This work investigated the impact of a quad screw [...] Read more.
During mechanical recycling, polypropylene typically is reprocessed using a single- or twin-screw extruder. The degradation of polypropylene during this reprocessing reduces the polymer’s molecular weight and, consequently, limits the performance of the recycled resin. This work investigated the impact of a quad screw extruder (QSE), which has greater free volume, on the reprocessing of an impact copolymer polypropylene. To mimic the recycling process, the polypropylene was subjected to three processing cycles using a QSE and a comparable twin-screw extruder (TSE) operated at three screw speeds. The reprocessed materials were characterized for their rheological, morphological, and mechanical properties. For both extruders, increasing the number of reprocessing cycles and the screw speed resulted in higher melt flow indices, decreases in zero-shear viscosity, and shifting of the crossover points for the storage and loss moduli, which indicate reductions in the molecular weight and narrowing of the molecular weight distribution of the polypropylene. The QSE exhibited greater reductions in molecular weight compared to the TSE, probably due to the higher stresses associated with the three intermeshing points along its screws. Reprocessing caused a significant reductions in the Izod impact strength of the reprocessed polypropylene, which correlated with reductions in the particle size and particle size distribution of the dispersed rubbery phase in the polypropylene during reprocessing. Full article
(This article belongs to the Special Issue Advanced Recycling of Plastic Waste: An Approach for Circular Economy)
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18 pages, 3972 KiB  
Article
Recyclability of Opaque PET from High Speed Melt Spinning: Determination of the Structures and Properties of Filaments
by Félix Odet, Noëllie Ylla, René Fulchiron and Philippe Cassagnau
Polymers 2022, 14(11), 2235; https://doi.org/10.3390/polym14112235 - 31 May 2022
Cited by 3 | Viewed by 2161
Abstract
Recycling opaque Polyethylene terephthalate (PET), which contains 1 to 10 wt % TiO2 submicron particles, has become of interest in the past few years. However, the bottle-to-fiber recyclability of opaque PET has not been assessed yet. In this work, opaque PET packaging [...] Read more.
Recycling opaque Polyethylene terephthalate (PET), which contains 1 to 10 wt % TiO2 submicron particles, has become of interest in the past few years. However, the bottle-to-fiber recyclability of opaque PET has not been assessed yet. In this work, opaque PET packaging has been characterized, and high-speed melt-spun filaments with different amounts of opaque PET (30–50–100%) blended with standard transparent recycled PET (rPET) have been produced in a pilot system. The opaque PET filaments produced have also been compared to a transparent rPET blend with masterbatch PET/TiO2 at different amounts of filler (1–3–6 wt %), produced with the same parameters. The structure-properties relationship of rPET melt-spun fibers has been investigated with crystallinity measurements, amorphous and crystalline phases orientation, and tenacity. It has been observed that the degree of crystallinity, the crystalline and amorphous phases orientation and the tenacity decreases with opaque PET addition and, to a lesser extent, with TiO2 addition. It has been suggested that TiO2 particles are not entirely responsible for the decrease in mechanical properties of opaque PET filaments since opaque rPET filaments have inferior properties to r-PET/TiO2 filaments at the same filler content. Full article
(This article belongs to the Special Issue Advanced Recycling of Plastic Waste: An Approach for Circular Economy)
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14 pages, 2911 KiB  
Article
Circular Economy Assessment in Recycling of LLDPE Bags According to European Resolution, Thermal and Structural Characterization
by Ricardo Ballestar, Celia Pradas, Fernando Carrillo-Navarrete, Javier Cañavate and Xavier Colom
Polymers 2022, 14(4), 754; https://doi.org/10.3390/polym14040754 - 15 Feb 2022
Cited by 3 | Viewed by 2406
Abstract
According to the Circular Economy Package promoted by the European directive, plastic bags companies must use in their formulations a percentage of polyethylene waste (industrial and/or domestic) greater than 70%. Following that regulation requires an understanding of its consequences in the final product [...] Read more.
According to the Circular Economy Package promoted by the European directive, plastic bags companies must use in their formulations a percentage of polyethylene waste (industrial and/or domestic) greater than 70%. Following that regulation requires an understanding of its consequences in the final product from an industrial point of view. This manuscript analyzes the thermal and morphological changes related to the tear resistance of linear-low density polyethylene (LLDPE) samples from industrial waste generated by the company Sphere Spain subjected to the degradation produced by the recycling cycles. The process is analogue to the industrial, starts from samples in pellets then a film by blow extrusion is obtained (odd steps) and posteriorly this film is recycled to pellets again (even steps). The results obtained show that the LLDPE samples develop two crystalline structures (CS1 and CS2) which evolve differently through the recycling cycles with a tendency to decrease in crystallinity due to degradation that is not the same for the process of obtaining film or recycling to pellet. The molecules with a more linear structure and a longer chain break and branch. The more branched structure increases and tends to crosslinking. This leads to a decrease in tear strength in the longitudinal direction, which is not so evident in the transversal direction. The samples could admit four recycling cycles with and acceptable tear resistance. The longitudinal tear strength value decreases by 40% for each film and 20% in the case of tearing in the transverse direction. The results obtained in this research work show that the regulations included in the cited circular economy package can be applied in the manufacture of consumer bags, helping also to reduce the dependence of manufacturers on fluctuations in delivery by collapses in shipping. Full article
(This article belongs to the Special Issue Advanced Recycling of Plastic Waste: An Approach for Circular Economy)
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Review

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35 pages, 4874 KiB  
Review
Improving Sustainability through Covalent Adaptable Networks in the Recycling of Polyurethane Plastics
by Edoardo Miravalle, Pierangiola Bracco, Valentina Brunella, Claudia Barolo and Marco Zanetti
Polymers 2023, 15(18), 3780; https://doi.org/10.3390/polym15183780 - 15 Sep 2023
Cited by 1 | Viewed by 1250
Abstract
The global plastic waste problem has created an urgent need for the development of more sustainable materials and recycling processes. Polyurethane (PU) plastics, which represent 5.5% of globally produced plastics, are particularly challenging to recycle owing to their crosslinked structure. Covalent adaptable networks [...] Read more.
The global plastic waste problem has created an urgent need for the development of more sustainable materials and recycling processes. Polyurethane (PU) plastics, which represent 5.5% of globally produced plastics, are particularly challenging to recycle owing to their crosslinked structure. Covalent adaptable networks (CANs) based on dynamic covalent bonds have emerged as a promising solution for recycling PU waste. CANs enable the production of thermoset polymers that can be recycled using methods that are traditionally reserved for thermoplastic polymers. Reprocessing using hot-pressing techniques, in particular, proved to be more suited for the class of polyurethanes, allowing for the efficient recycling of PU materials. This Review paper explores the potential of CANs for improving the sustainability of PU recycling processes by examining different types of PU-CANs, bond types, and fillers that can be used to optimise the recycling efficiency. The paper concludes that further research is needed to develop more cost-effective and industrial-friendly techniques for recycling PU-CANs, as they can significantly contribute to sustainable development by creating recyclable thermoset polymers. Full article
(This article belongs to the Special Issue Advanced Recycling of Plastic Waste: An Approach for Circular Economy)
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23 pages, 5297 KiB  
Review
A Thermo-Catalytic Pyrolysis of Polystyrene Waste Review: A Systematic, Statistical, and Bibliometric Approach
by Arantxa M. Gonzalez-Aguilar, Vicente Pérez-García and José M. Riesco-Ávila
Polymers 2023, 15(6), 1582; https://doi.org/10.3390/polym15061582 - 22 Mar 2023
Cited by 5 | Viewed by 2876
Abstract
Global polystyrene (PS) production has been influenced by the lightness and heat resistance this material offers in different applications, such as construction and packaging. However, population growth and the lack of PS recycling lead to a large waste generation, affecting the environment. Pyrolysis [...] Read more.
Global polystyrene (PS) production has been influenced by the lightness and heat resistance this material offers in different applications, such as construction and packaging. However, population growth and the lack of PS recycling lead to a large waste generation, affecting the environment. Pyrolysis has been recognized as an effective recycling method, converting PS waste into valuable products in the chemical industry. The present work addresses a systematic, bibliometric, and statistical analysis of results carried out from 2015 to 2022, making an extensive critique of the most influential operation parameters in the thermo-catalytic pyrolysis of PS and its waste. The systematic study showed that the conversion of PS into a liquid with high aromatic content (84.75% of styrene) can be achieved by pyrolysis. Discussion of PS as fuel is described compared to commercial fuels. In addition, PS favors the production of liquid fuel when subjected to co-pyrolysis with biomass, improving its properties such as viscosity and energy content. A statistical analysis of the data compilation was also discussed, evaluating the influence of temperature, reactor design, and catalysts on product yield. Full article
(This article belongs to the Special Issue Advanced Recycling of Plastic Waste: An Approach for Circular Economy)
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23 pages, 4035 KiB  
Review
Plastic Waste Upcycling: A Sustainable Solution for Waste Management, Product Development, and Circular Economy
by Rajkamal Balu, Naba Kumar Dutta and Namita Roy Choudhury
Polymers 2022, 14(22), 4788; https://doi.org/10.3390/polym14224788 - 08 Nov 2022
Cited by 22 | Viewed by 9290
Abstract
Plastic waste pollution, including non-biodegradable landfills, leaching of toxic chemicals into soil and waterways, and emission of toxic gases into the atmosphere, is significantly affecting our environment. Conventional plastic waste recycling approaches generally produce lower value materials compared to the original plastic or [...] Read more.
Plastic waste pollution, including non-biodegradable landfills, leaching of toxic chemicals into soil and waterways, and emission of toxic gases into the atmosphere, is significantly affecting our environment. Conventional plastic waste recycling approaches generally produce lower value materials compared to the original plastic or recover inefficient heat energy. Lately, upcycling or the valorization approach has emerged as a sustainable solution to transform plastic waste into value-added products. In this review, we present an overview of recent advancements in plastic waste upcycling, such as vitrimerization, nanocomposite fabrication, additive manufacturing, catalytic transformation, and industrial biotechnology, envisaged with technical challenges, future developments, and new circular economy opportunities. Full article
(This article belongs to the Special Issue Advanced Recycling of Plastic Waste: An Approach for Circular Economy)
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