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1.
Chemosphere ; 350: 141069, 2024 Feb.
Article in English | MEDLINE | ID: mdl-38160949

ABSTRACT

Deodorization and, in a broader sense, the removal of volatile organic compounds (VOCs) from plastic waste have become increasingly important in the field of plastic recycling, and various new decontamination techniques have been developed. Both in research and industrial practice, the selection of VOCs has been random or unsubstantiated, making it difficult to compare studies and assess decontamination processes objectively. Thus, this study proposes the use of Statistical Molecular Design (SMD) and Quantitative Structure - Activity Relationship (QSAR) as chemometric tools for the selection of representative VOCs, based on physicochemical properties. Various algorithms are used for SMD; hence, several frequently used D-Optimal Onion Design (DOOD) and Space-Filling (SF) algorithms were assessed. Hereby, it was validated that DOOD, by dividing the layers based on the equal-distance approach without so-called 'Adjacent Layer Bias', results in the most representative selection of VOCs. QSAR models that describe VOC removal by water-based washing of plastic waste as a function of molecular weight, polarizability, dipole moment and Hansen Solubility Parameters Distance were successfully established. An adjusted-R2 value of 0.77 ± 0.09 and a mean absolute error of 24.5 ± 4 % was obtained. Consequently, by measuring a representative selection of VOCs compiled using SMD, the removal of other unanalyzed VOCs was predicted on the basis of the QSAR. Another advantage of the proposed chemometric selection procedure is its flexibility. SMD allows to extend or modify the considered dataset according to the available analytical techniques, and to adjust the considered physicochemical properties according to the intended process.


Subject(s)
Volatile Organic Compounds , Quantitative Structure-Activity Relationship , Chemometrics
2.
J Hazard Mater ; 452: 131239, 2023 Jun 15.
Article in English | MEDLINE | ID: mdl-36963193

ABSTRACT

Plastic packaging is usually heavily printed with inks to provide functional benefits. However, the presence of inks strongly impedes the closed-loop recycling of plastic films. Various media have already been studied for the deinking of plastic films, but there is little scientific insight into the effectiveness of different deinking techniques. Therefore, this study aims to obtain a systematic understanding by measuring the liquefaction and maximum solubility of 14 chemically different polymer resins in seven different media typically used in plastic deinking, such as acetone, ethyl acetate, sodium hydroxide solution, cetyltrimethylammonium bromide solution, formic acid, sulfuric acid, and N,N-dimethylcyclohexylamine. Our findings show that acid-based media are able to remove a broader range of polymer resins. Organic solvents are particularly effective against acrylics and related polymer resins. The deinking efficiency tests on pure resins are also confirmed by deinking four printed plastic films containing different classes of polymer resins. A basic cost and environmental impact analysis is given to evaluate scale-up potential of the deinking medium.

3.
Ind Eng Chem Res ; 61(30): 10999-11011, 2022 Aug 03.
Article in English | MEDLINE | ID: mdl-35941852

ABSTRACT

The viscosity of polymer solutions is important for both polymer synthesis and recycling. Polymerization reactions can become hampered by diffusional limitations once a viscosity threshold is reached, and viscous solutions complicate the cleaning steps during the dissolution-precipitation technique. Available experimental data is limited, which is more severe for green solvents, justifying dedicated viscosity data recording and interpretation. In this work, a systematic study is therefore performed on the viscosity of polystyrene solutions, considering different concentrations, temperatures, and conventional and green solvents. The results show that for the shear rate range of 1-1000 s-1, the solutions with concentrations between 5 and 39 wt % display mainly Newtonian behavior, which is further confirmed by the applicability of the segment-based Eyring-NRTL and Eyring-mNRF models. Moreover, multivariate data analysis successfully predicts the viscosity of polystyrene solutions under different conditions. This approach will facilitate future data recording for other polymer-solvent combinations while minimizing experimental effort.

4.
Sci Total Environ ; 812: 152467, 2022 Mar 15.
Article in English | MEDLINE | ID: mdl-34952061

ABSTRACT

An important impediment to the acceptance of recyclates into a broader market is their unwanted odor after reprocessing. Different types of washing procedures are already in place, but fundamental insights into the deodorization efficiencies of different washing media are still relatively scarce. Therefore, in this study, the deodorization efficiencies of different types of plastics after washing with different media were determined via gas chromatography and mass spectrometry analysis. A total of 169 compounds subdivided into various chemical classes, such as alkanes, terpenes, and oxygenated compounds, were detected across all packaging types. Around 60 compounds were detected on plastic bottles, and around 40 were detected on trays and films. Owing to the differences in physicochemical properties of odor compounds, different deodorization efficiencies were obtained with different washing media. Water and caustic soda were significantly more efficient for poly(ethylene terephthalate) bottles with deodorization efficiencies up to 80%, whereas for polyethylene (PE) and polypropylene bottles, the washing media were relatively inefficient (around 30-40%). Adding a detergent or an organic solvent could increase deodorization efficiencies by up to 70-90% for these packaging types. A similar trend was observed for PE films having deodorization efficiencies in the range of 40-50% when washing with water or caustic soda and around 70-80% when a detergent was added. Polystyrene trays were most effectively deodorized with a detergent, achieving efficiencies up to 67%. Hence, this study shows that optimal washing processes should be tailored to specific packaging types to further improve deodorization and to eventually be able to meet ambitious European recycling targets.


Subject(s)
Plastics , Recycling , Gas Chromatography-Mass Spectrometry , Polyethylene , Polyethylene Terephthalates
5.
ChemSusChem ; 14(19): 4071-4102, 2021 Oct 05.
Article in English | MEDLINE | ID: mdl-34324273

ABSTRACT

Solvent-based recycling is a promising approach for closed-loop recovery of plastic-containing waste. It avoids the energy cost to depolymerize the plastic but still allows to clean the polymer of contaminants and additives. However, viscosity plays an important role in handling the polymer solutions at high concentrations and in the cleaning steps. This Review addresses the viscosity behavior of polymer solutions, available data, and (mostly algebraic) models developed. The non-Newtonian viscosity models, such as the Carreau and Yasuda-Cohen-Armstrong models, pragmatically describe the viscosity of polymer solutions at different concentrations and shear rate ranges. This Review also describes how viscosity influences filtration and centrifugation processes, which are crucial steps in the cleaning of the polymer and includes a polystyrene/styrene case study.

6.
ChemSusChem ; 14(19): 4198-4213, 2021 Oct 05.
Article in English | MEDLINE | ID: mdl-33492767

ABSTRACT

Recycling multilayer plastic packaging is challenging due to its intrinsic compositional heterogeneity. A promising route to increase recycling rates for these materials is delamination, which allows recycling the polymers separately. Yet, this process is not well understood on a fundamental level. This study aimed to obtain first principles-based insights of the delamination mechanism of multilayer flexible packaging film (MFPF) with carboxylic acids. Delamination of MFPFs was described through a model based on Fick's first law of diffusion and first-order dissolution kinetics of polyurethane adhesives. The model was experimentally tested on 5 different MFPFs at different temperatures (50-75 °C), formic acid concentrations (50-100 vol %), and solid/liquid (S/L) ratios (0.005, 0.025, and 0.12 g mL-1 ). Under the studied conditions the model proved to successfully estimate the delamination time of MFPF with the average Theil's Inequality Coefficient (TIC) value of 0.14. Essential for scaling-up delamination processes is the possibility to use high S/L ratios as the solubility of the adhesive is rarely limiting.

7.
Waste Manag ; 120: 564-575, 2021 Feb 01.
Article in English | MEDLINE | ID: mdl-33139193

ABSTRACT

Mechanical recycling is to date the most commonly applied recycling technology. However, mechanical recycling of post-consumer plastics still faces many challenges, such as the presence of odorous constituents. Accordingly, recycling industry is looking for cost-effective solutions to improve the current washing efficiencies. However, scientific literature and basic understanding of deodorization processes are still scarce, which impedes efficient industrial optimization. Therefore, this study aims to obtain more fundamental insights in the deodorization mechanisms of plastic films in different washing media such as water, detergent, caustic soda, and ethyl acetate as organic solvent. The removal efficiencies of 19 odor components with a wide range of physicochemical properties were quantified via GC-MS analysis. The results revealed that deodorization depends on various factors such as temperature and physicochemical properties as polarity, volatility, and molecular weight of the odor components and the washing media. It was shown that polar washing media are less efficient compared to apolar media or media containing a detergent, achieving efficiencies of around 50% and 90%, respectively. The desorption processes can be accurately modeled by the isotherm model of Fritz-Schlunder in combination with a reversible first order kinetic model for the deodorization kinetics. Aspen Plus® process simulations of a water-based washing process reveal that at least 60% fresh water is needed to avoid saturation of the medium and undesired (re-)adsorption of odor components onto the plastics, which results in a substantial ecological footprint.


Subject(s)
Odorants , Plastics , Gas Chromatography-Mass Spectrometry , Kinetics , Recycling
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