Advances in Biodegradation of Plastics

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 (10 March 2023) | Viewed by 74481

Special Issue Editors


E-Mail Website
Guest Editor
Department of Chemistry and Bioscience, Aalborg University, Fredrik Bajers Vej 7H, 9220 Aalborg, Denmark
Interests: chemistry and bioscience; fermentation technology; biorefinery; plastic biodegradation; waste valorization
Special Issues, Collections and Topics in MDPI journals

E-Mail Website
Guest Editor
Department for Agrobiotechnology, IFA-Tulln, Institute for Environmental Biotechnology, University of Natural Resources and Life Sciences, Vienna, Konrad Lorenz Strasse 20, A-3430 Tulln an der Donau, Austria
Interests: chemo-enzymatic processing of polymers and materials; plastic recycling; circular materials; surface functionalization

Special Issue Information

Dear Colleagues,

According to the Ellen McArthur Report 2020, up to 9 million tons of plastic waste leak into the oceans each year, feeding the big garbage patches. Sadly, by 2050, there might be as much (micro)plastics as fish biomass in the sea. How did we get to this?

With a global production of 350 million tons in 2018 and a 4-fold increase foreseen in the next 30 years, plastic is becoming one of the most abundant anthropogenic materials, with multiple implications on economy and environment. Moreover, due to inefficient waste management, recycling rates of post-consumer plastics only reach a disappointing 14% worldwide. Most plastic waste ends up incinerated and landfilled, while only a minor fraction is collected for recycling.

The low rates of recycling have made plastic pollution one of the biggest waste problems faced by today’s society. In fact, relevant fractions of plastic cannot be (economically) recycled with conventional technologies, and new solutions are urgently needed. In addition to mechanical and chemical recycling, new studies are now investigating biochemical recycling routes, mainly through enzyme technology and protein engineering. These technologies might represent a much-needed cornerstone for a more circular use of plastic and have the potential to complement the already existing technologies, by targeting the currently non-recycled fractions. However, the hydrophobicity and high crystallinity of plastics are still of major concern, often leading to slow kinetics and incomplete degradation, thus requiring further research and process optimization. For this reason, biotechnological plastic degradation and recycling are often overlooked on an industrial level, even though a new biotechnology by Carbios and Toulouse White Biotechnology allows obtaining efficient depolymerization of poly(ethylene terephthalate) on an industry-relevant scale and processing time. Considering that biotechnological degradation of plastics is still at a very early stage, these results are very promising and stimulate further research and development.

Relevant Literature:

- Ellen McArtur Foundation, Breaking the Wave: A Comprehensive Assessment of Pathways Towards Stopping Ocean Plastic Pollution, 2020;

- R. Wei, et al., Possibilities and limitations of biotechnological plastic degradation and recycling, Nat. Catal. 3 (2020) 867–871;

- E. Guémard, et al., An engineered PET depolymerase to break down and recycle plastic bottles, Nature. 580 (2020)

Dr. Cristiano Varrone
Dr. Alessandro Pellis
Guest Editors

Manuscript Submission Information

Manuscripts should be submitted online at www.mdpi.com by registering and logging in to this website. Once you are registered, click here to go to the submission form. Manuscripts can be submitted until the deadline. All submissions that pass pre-check are peer-reviewed. Accepted papers will be published continuously in the journal (as soon as accepted) and will be listed together on the special issue website. Research articles, review articles as well as short communications are invited. For planned papers, a title and short abstract (about 100 words) can be sent to the Editorial Office for announcement on this website.

Submitted manuscripts should not have been published previously, nor be under consideration for publication elsewhere (except conference proceedings papers). All manuscripts are thoroughly refereed through a single-blind peer-review process. A guide for authors and other relevant information for submission of manuscripts is available on the Instructions for Authors page. Polymers is an international peer-reviewed open access semimonthly journal published by MDPI.

Please visit the Instructions for Authors page before submitting a manuscript. The Article Processing Charge (APC) for publication in this open access journal is 2700 CHF (Swiss Francs). Submitted papers should be well formatted and use good English. Authors may use MDPI's English editing service prior to publication or during author revisions.

Keywords

  • Plastic waste
  • Biodegradation
  • Recycling
  • Bio-upcycling
  • Post-consumer plastic
  • End-of-life
  • Eco-design
  • Circular bioeconomy
  • Computational studies

Published Papers (17 papers)

Order results
Result details
Select all
Export citation of selected articles as:

Research

Jump to: Review

18 pages, 4006 KiB  
Article
Effect of the Presence of Lignin from Woodflour on the Compostability of PHA-Based Biocomposites: Disintegration, Biodegradation and Microbial Dynamics
by Patricia Feijoo, Anna Marín, Kerly Samaniego-Aguilar, Estefanía Sánchez-Safont, José M. Lagarón, José Gámez-Pérez and Luis Cabedo
Polymers 2023, 15(11), 2481; https://doi.org/10.3390/polym15112481 - 27 May 2023
Cited by 4 | Viewed by 1763
Abstract
Poly(3-hydroxybutyrate-co-3-hydroxyvalerate) (PHBV) has gained attention as a possible substitute for conventional polymers that could be integrated into the organic recycling system. Biocomposites with 15% of pure cellulose (TC) and woodflour (WF) were prepared to analyze the role of lignin on their [...] Read more.
Poly(3-hydroxybutyrate-co-3-hydroxyvalerate) (PHBV) has gained attention as a possible substitute for conventional polymers that could be integrated into the organic recycling system. Biocomposites with 15% of pure cellulose (TC) and woodflour (WF) were prepared to analyze the role of lignin on their compostability (58 °C) by tracking the mass loss, CO2 evolution, and the microbial population. Realistic dimensions for typical plastic products (400 µm films), as well as their service performance (thermal stability, rheology), were taken into account in this hybrid study. WF showed lower adhesion with the polymer than TC and favored PHBV thermal degradation during processing, also affecting its rheological behavior. Although all materials disintegrated in 45 days and mineralized in less than 60 days, lignin from woodflour was found to slow down the bioassimilation of PHBV/WF by limiting the access of enzymes and water to easier degradable cellulose and polymer matrix. According to the highest and the lowest weight loss rates, TC incorporation allowed for higher mesophilic bacterial and fungal counts, while WF seemed to hinder fungal growth. At the initial steps, fungi and yeasts seem to be key factors in facilitating the later metabolization of the materials by bacteria. Full article
(This article belongs to the Special Issue Advances in Biodegradation of Plastics)
Show Figures

Graphical abstract

18 pages, 10328 KiB  
Article
Spectrophotometric-Based Assay to Quantify Relative Enzyme-Mediated Degradation of Commercially Available Bioplastics
by Matthew Hoekstra and Myron L. Smith
Polymers 2023, 15(11), 2439; https://doi.org/10.3390/polym15112439 - 24 May 2023
Cited by 1 | Viewed by 2232
Abstract
We present a spectrophotometric-based assay to identify enzymes that degrade commercially available bioplastics. Bioplastics comprise aliphatic polyesters with hydrolysis-susceptible ester bonds and are proposed as a replacement for petroleum-based plastics that accumulate in the environment. Unfortunately, many bioplastics can also persist in environments [...] Read more.
We present a spectrophotometric-based assay to identify enzymes that degrade commercially available bioplastics. Bioplastics comprise aliphatic polyesters with hydrolysis-susceptible ester bonds and are proposed as a replacement for petroleum-based plastics that accumulate in the environment. Unfortunately, many bioplastics can also persist in environments including seawater and waste centers. Our assay involves an overnight incubation of candidate enzyme(s) with plastic, followed by A610 spectrophotometry using 96-well plates to quantify both a reduction in residual plastic and the liberation of degradation by-products. We use the assay to show that Proteinase K and PLA depolymerase, two enzymes that were previously shown to degrade pure polylactic acid plastic, promote a 20–30% breakdown of commercial bioplastic during overnight incubation. We validate our assay and confirm the degradation potential of these enzymes with commercial bioplastic using established mass-loss and scanning electron microscopy methods. We show how the assay can be used to optimize parameters (temperature, co-factors, etc.) to enhance the enzyme-mediated degradation of bioplastics. The assay endpoint products can be coupled with nuclear magnetic resonance (NMR) or other analytical methods to infer the mode of enzymatic activity. Overall, the screening capacity of the spectrophotometric-based assay was demonstrated to be an accurate method to identify bioplastic-degrading enzymes. Full article
(This article belongs to the Special Issue Advances in Biodegradation of Plastics)
Show Figures

Figure 1

17 pages, 5751 KiB  
Article
A New Colorimetric Test for Accurate Determination of Plastic Biodegradation
by Valérie Mattelin, Lennert Verfaille, Kankana Kundu, Stefaan De Wildeman and Nico Boon
Polymers 2023, 15(10), 2311; https://doi.org/10.3390/polym15102311 - 15 May 2023
Viewed by 1525
Abstract
As plastic waste is accumulating in both controlled waste management settings and natural settings, much research is devoted to search for solutions, also in the field of biodegradation. However, determining the biodegradability of plastics in natural environments remains a big challenge due to [...] Read more.
As plastic waste is accumulating in both controlled waste management settings and natural settings, much research is devoted to search for solutions, also in the field of biodegradation. However, determining the biodegradability of plastics in natural environments remains a big challenge due to the often very low biodegradation rates. Many standardised test methods for biodegradation in natural environments exist. These are often based on mineralisation rates in controlled conditions and are thus indirect measurements of biodegradation. It is of interest for both researchers and companies to have tests that are more rapid, easier, and more reliable to screen different ecosystems and/or niches for their plastic biodegradation potential. In this study, the goal is to validate a colorimetric test, based on carbon nanodots, to screen biodegradation of different types of plastics in natural environments. After introducing carbon nanodots into the matrix of the target plastic, a fluorescent signal is released upon plastic biodegradation. The in-house-made carbon nanodots were first confirmed regarding their biocompatibility and chemical and photostability. Subsequently, the effectivity of the developed method was evaluated positively by an enzymatic degradation test with polycaprolactone with Candida antarctica lipase B. Finally, validation experiments were performed with enriched microorganisms and real environmental samples (freshwater and seawater), of which the results were compared with parallel, frequently used biodegradation measures such as O2 and CO2, dissolved organic carbon, growth and pH, to assess the reliability of the test. Our results indicate that this colorimetric test is a good alternative to other methods, but a combination of different methods gives the most information. In conclusion, this colorimetric test is a good fit to screen, in high throughput, the depolymerisation of plastics in natural environments and under different conditions in the lab. Full article
(This article belongs to the Special Issue Advances in Biodegradation of Plastics)
Show Figures

Graphical abstract

24 pages, 6728 KiB  
Article
Fungal Screening for Potential PET Depolymerization
by Lusiane Malafatti-Picca, Elaine Cristina Bucioli, Michel Ricardo de Barros Chaves, Aline Machado de Castro, Érika Valoni, Valéria Maia de Oliveira, Anita Jocelyne Marsaioli, José Silvio Govone, Dejanira de Franceschi de Angelis, Michel Brienzo and Derlene Attili-Angelis
Polymers 2023, 15(6), 1581; https://doi.org/10.3390/polym15061581 - 22 Mar 2023
Cited by 3 | Viewed by 2283
Abstract
Approximately 400 billion PET bottles are produced annually in the world, of which from 8 to 9 million tons are discarded in oceans. This requires developing strategies to urgently recycle them. PET recycling can be carried out using the microbial hydrolysis of polymers [...] Read more.
Approximately 400 billion PET bottles are produced annually in the world, of which from 8 to 9 million tons are discarded in oceans. This requires developing strategies to urgently recycle them. PET recycling can be carried out using the microbial hydrolysis of polymers when monomers and oligomers are released. Exploring the metabolic activity of fungi is an environmentally friendly way to treat harmful polymeric waste and obtain the production of monomers. The present study addressed: (i) the investigation of potential of strains with the potential for the depolymerization of PET bottles from different manufacturers (crystallinity of 35.5 and 10.4%); (ii) the search for a culture medium that favors the depolymerization process; and (iii) gaining more knowledge on fungal enzymes that can be applied to PET recycling. Four strains (from 100 fungal strains) were found as promising for conversion into terephthalic acid from PET nanoparticles (npPET): Curvularia trifolii CBMAI 2111, Trichoderma sp. CBMAI 2071, Trichoderma atroviride CBMAI 2073, and Cladosporium cladosporioides CBMAI 2075. The fermentation assays in the presence of PET led to the release of terephthalic acid in concentrations above 12 ppm. Biodegradation was also confirmed using mass variation analyses (reducing mass), scanning electron microscopy (SEM) that showed evidence of material roughness, FTIR analysis that showed band modification, enzymatic activities detected for lipase, and esterase and cutinase, confirmed by monomers/oligomers quantification using high performance liquid chromatography (HPLC-UV). Based on the microbial strains PET depolymerization, the results are promising for the exploration of the selected microbial strain. Full article
(This article belongs to the Special Issue Advances in Biodegradation of Plastics)
Show Figures

Figure 1

12 pages, 1570 KiB  
Article
Computational Exploration of Bio-Degradation Patterns of Various Plastic Types
by Sunny Malik, Ankita Maurya, Sunil Kumar Khare and Kinshuk Raj Srivastava
Polymers 2023, 15(6), 1540; https://doi.org/10.3390/polym15061540 - 20 Mar 2023
Cited by 5 | Viewed by 2057
Abstract
Plastic materials are recalcitrant in the open environment, surviving for longer without complete remediation. The current disposal methods of used plastic material are inefficient; consequently, plastic wastes are infiltrating the natural resources of the biosphere. The mixed composition of urban domestic waste with [...] Read more.
Plastic materials are recalcitrant in the open environment, surviving for longer without complete remediation. The current disposal methods of used plastic material are inefficient; consequently, plastic wastes are infiltrating the natural resources of the biosphere. The mixed composition of urban domestic waste with different plastic types makes them unfavorable for recycling; however, natural assimilation in situ is still an option to explore. In this research work, we have utilized previously published reports on the biodegradation of various plastics types and analyzed the pattern of microbial degradation. Our results demonstrate that the biodegradation of plastic material follows the chemical classification of plastic types based on their main molecular backbone. The clustering analysis of various plastic types based on their biodegradation reports has grouped them into two broad categories of C-C (non-hydrolyzable) and C-X (hydrolyzable). The C-C and C-X groups show a statistically significant difference in their biodegradation pattern at the genus level. The Bacilli class of bacteria is found to be reported more often in the C-C category, which is challenging to degrade compared to C-X. Genus enrichment analysis suggests that Pseudomonas and Bacillus from bacteria and Aspergillus and Penicillium from fungi are potential genera for the bioremediation of mixed plastic waste. The lack of uniformity in reporting the results of microbial degradation of plastic also needs to be addressed to enable productive growth in the field. Overall, the result points towards the feasibility of a microbial-based biodegradation solution for mixed plastic waste. Full article
(This article belongs to the Special Issue Advances in Biodegradation of Plastics)
Show Figures

Graphical abstract

16 pages, 1959 KiB  
Article
Polyurethane Foam Waste Upcycling into an Efficient and Low Pollutant Gasification Syngas
by Rezgar Hasanzadeh, Parisa Mojaver, Shahram Khalilarya, Taher Azdast, Ata Chitsaz and Mehran Mojaver
Polymers 2022, 14(22), 4938; https://doi.org/10.3390/polym14224938 - 15 Nov 2022
Cited by 8 | Viewed by 1254
Abstract
Waste treatment has attracted much attention and, in this regard, gasification processes offer an efficient thermochemical technique that can produce a syngas rich in hydrogen. This technique has been well developed for solid waste and biomass while investigations on gasification of polymeric foam [...] Read more.
Waste treatment has attracted much attention and, in this regard, gasification processes offer an efficient thermochemical technique that can produce a syngas rich in hydrogen. This technique has been well developed for solid waste and biomass while investigations on gasification of polymeric foam are rare. Therefore, this study explores the treatment of polyurethane foam waste with different gasifying agents, based on thermodynamic modeling. The polymeric foam gasification was developed using the best model for estimating higher heating value (gross calorific value). As the results indicated, models based on both ultimate and proximate analyses had better performance in predicting higher heating value. As one of the main objectives and novelties, the steam and air gasification performance of flexible and rigid polyurethane foam wastes was investigated and compared from efficiency and CO2 emission viewpoints. Polyurethane foam gasification by steam resulted in higher hydrogen efficiency, led to lower energy efficiency and produced lower CO2 emissions compared to gasification by air. A hydrogen efficiency of 41.4% was obtained for gasification of waste flexible polyurethane foam by steam. An energy efficiency of 76.6% and CO2 emission of 7.43 g per mole of feedstock were attained for waste flexible polyurethane foam gasified by air. Full article
(This article belongs to the Special Issue Advances in Biodegradation of Plastics)
Show Figures

Figure 1

16 pages, 3856 KiB  
Article
Polypropylene Recovery and Recycling from Mussel Nets
by Loris Pietrelli
Polymers 2022, 14(17), 3469; https://doi.org/10.3390/polym14173469 - 25 Aug 2022
Cited by 2 | Viewed by 1647
Abstract
Mussels represent about one-third of all aquaculture products sold in the European Union. Theoretically, mussel production should be an environmentally friendly and sustainable activity (0.252 kg CO2 eq. per 1 kg of mussel produced against over 20 kg CO2 eq. per [...] Read more.
Mussels represent about one-third of all aquaculture products sold in the European Union. Theoretically, mussel production should be an environmentally friendly and sustainable activity (0.252 kg CO2 eq. per 1 kg of mussel produced against over 20 kg CO2 eq. per 1 kg of beef produced) but the abandoned plastic “socks” on the seabed and along beaches represent a significant environmental problem. The recovery and recycling of those polymer materials represents the proper management of the waste issue due to mussel farming. This study was performed to investigate, for the first time, the roles of the chemical oxidation actions on the detachment (and destruction) of organic matter (biofilm in particular) from the surface of the polypropylene “socks” used in sea farms in order to recover the polymer material and recycle it. In the experiments, oxidation by H2O2 and HNO3 was performed on the studied samples. The effects of the particle size of the fragments, oxidant concentration, agitation time and ultrasound application were determined. FTIR spectra and tensile mechanical properties of the samples after treatment were measured and compared with the virgin polymer material. The biodiversity and structure of the plastic-associated biofilm was also determined before and after the oxidation process. Based on the results of the characterization of the recovered polymer material, a process scheme was designed. The application of the developed process could significantly reduce the environmental risk associated with used mussel socks. The One LIFE (the EU’s funding instrument for the environment and climate action) Project was recently founded based on this research. Full article
(This article belongs to the Special Issue Advances in Biodegradation of Plastics)
Show Figures

Graphical abstract

24 pages, 2612 KiB  
Article
Enzymatic Degradation of the Most Common Aliphatic Bio-Polyesters and Evaluation of the Mechanisms Involved: An Extended Study
by Antonella Rosato, Angela Romano, Grazia Totaro, Annamaria Celli, Fabio Fava, Giulio Zanaroli and Laura Sisti
Polymers 2022, 14(9), 1850; https://doi.org/10.3390/polym14091850 - 30 Apr 2022
Cited by 33 | Viewed by 4860
Abstract
Commercial hydrolytic enzymes belonging to different subclasses (several lipases, proteinase k, cutinase) were investigated for their ability to degrade different aliphatic polyesters, i.e., poly(butylene succinate) (PBS), poly(butylene succinate-co-adipate) (PBSA), two poly(caprolactone), having two different molecular weights, poly(lactic acid) (PLA) and poly(propylene [...] Read more.
Commercial hydrolytic enzymes belonging to different subclasses (several lipases, proteinase k, cutinase) were investigated for their ability to degrade different aliphatic polyesters, i.e., poly(butylene succinate) (PBS), poly(butylene succinate-co-adipate) (PBSA), two poly(caprolactone), having two different molecular weights, poly(lactic acid) (PLA) and poly(propylene carbonate) (PPC). The enzyme screening was first carried out by investigating the capacity of fully degrading the target polymers in 24 h, then weight loss measurements of selected polyesters and target enzymes were performed. Solid residues after enzyme degradation were characterized by proton nuclear magnetic resonance (1H NMR), gel permeation chromatography (GPC), infrared spectroscopy (FT-IR), differential scanning calorimetry (DSC) and thermogravimetry (TGA). Liquid fractions were studied via GPC, 1H NMR and high-performance liquid chromatography (HPLC). PCL and PBSA were found to be the most biodegradable polyesters, under the conditions used in this study. PBS was fully degraded only by cutinase, whereas none of the tested enzymes were able to completely degrade PLA and PPC, in the conditions assessed here. Cutinase exhibited the highest hydrolytic activity on PBSA, while lipase from Candida sp. (CALB) on low molecular weight PCL. Chemical analyses on residual solids showed that the enzymatic degradation occurred homogeneously from the surface through an erosion mechanism and did not significantly affect the macromolecular structure and thermal stability. Cleaving action mode for each enzyme (endo- and/or exo-type) on the different polyesters were also proposed based on the evaluation of the degradation products in the liquid fraction. Full article
(This article belongs to the Special Issue Advances in Biodegradation of Plastics)
Show Figures

Figure 1

12 pages, 2737 KiB  
Article
Properties and Degradability of Poly(Butylene Adipate-Co-Terephthalate)/Calcium Carbonate Films Modified by Polyethylene Glycol
by Xiaoqian Diao, Caili Zhang and Yunxuan Weng
Polymers 2022, 14(3), 484; https://doi.org/10.3390/polym14030484 - 26 Jan 2022
Cited by 14 | Viewed by 4072
Abstract
Poly(butylene adipate-co-terephthalate) (PBAT) is a biodegradable polymer synthesized from petrochemical resources. PBAT has an exceptionally high elongation at break values which makes it one of the most promising substitutes for LDPE packaging films. However, the applicability of PBAT films is still limited by [...] Read more.
Poly(butylene adipate-co-terephthalate) (PBAT) is a biodegradable polymer synthesized from petrochemical resources. PBAT has an exceptionally high elongation at break values which makes it one of the most promising substitutes for LDPE packaging films. However, the applicability of PBAT films is still limited by low strength and high production costs. In this work, we used polyethylene glycol 600 (PEG-600) as a coating agent to modify the surface of calcium carbonate and improve compatibility with the polymer matrix. A series of PBAT/CaCO3 composite films having different CaCO3 particle size and content of coating agent was prepared using extrusion blow molding. The effect of particle size of CaCO3 filler and the content of a coating agent on the mechanical and rheological properties of composite films have been studied. The biodegradation properties have been tested by burying the samples in soil or keeping them in artificial seawater for 90 days. It was shown that the addition of PEG-600 improves compatibility between the matrix and CaCO3 filler as polar –OH groups of PEG have a high affinity toward the polar surface of CaCO3. Moreover, the hydrophilicity of PEG-600 increased the diffusivity of water molecules and facilitated PBAT degradation. This work provides experimental data and theoretical guidance that support the development of high-performance PBAT/calcium carbonate films for the single use packaging industry. Full article
(This article belongs to the Special Issue Advances in Biodegradation of Plastics)
Show Figures

Figure 1

12 pages, 2299 KiB  
Article
Cutinase-Catalyzed Polyester-Polyurethane Degradation: Elucidation of the Hydrolysis Mechanism
by Federico Di Bisceglie, Felice Quartinello, Robert Vielnascher, Georg M. Guebitz and Alessandro Pellis
Polymers 2022, 14(3), 411; https://doi.org/10.3390/polym14030411 - 20 Jan 2022
Cited by 17 | Viewed by 4779
Abstract
Polyurethanes (PU) are one of the most-used classes of synthetic polymers in Europe, having a considerable impact on the plastic waste management in the European Union. Therefore, they represent a major challenge for the recycling industry, which requires environmentally friendly strategies to be [...] Read more.
Polyurethanes (PU) are one of the most-used classes of synthetic polymers in Europe, having a considerable impact on the plastic waste management in the European Union. Therefore, they represent a major challenge for the recycling industry, which requires environmentally friendly strategies to be able to re-utilize their monomers without applying hazardous and polluting substances in the process. In this work, enzymatic hydrolysis of a polyurethane-polyester (PU-PE) copolymer using Humicola insolens cutinase (HiC) has been investigated in order to achieve decomposition at milder conditions and avoiding harsh chemicals. PU-PE films have been incubated with the enzyme at 50 °C for 168 h, and hydrolysis has been followed throughout the incubation. HiC effectively hydrolysed the polymer, reducing the number average molecular weight (Mn) and the weight average molecular weight (Mw) by 84% and 42%, respectively, as shown by gel permeation chromatography (GPC), while scanning electron microscopy showed cracks at the surface of the PU-PE films as a result of enzymatic surface erosion. Furthermore, Fourier Transform Infrared (FTIR) analysis showed a reduction in the peaks at 1725 cm−1, 1164 cm−1 and 1139 cm−1, indicating that the enzyme preferentially hydrolysed ester bonds, as also supported by the nuclear magnetic resonance spectroscopy (NMR) results. Liquid chromatography time-of-flight/mass spectrometry (LC-MS-Tof) analysis revealed the presence in the incubation supernatant of all of the monomeric constituents of the polymer, thus suggesting that the enzyme was able to hydrolyse both the ester and the urethane bonds of the polymer. Full article
(This article belongs to the Special Issue Advances in Biodegradation of Plastics)
Show Figures

Graphical abstract

11 pages, 680 KiB  
Article
Rational Protein Engineering to Increase the Activity and Stability of IsPETase Using the PROSS Algorithm
by Andrew Rennison, Jakob R. Winther and Cristiano Varrone
Polymers 2021, 13(22), 3884; https://doi.org/10.3390/polym13223884 - 10 Nov 2021
Cited by 16 | Viewed by 4407
Abstract
Polyethylene terephthalate (PET) is the most widely used polyester plastic, with applications in the textile and packaging industry. Currently, re-moulding is the main path for PET recycling, but this eventually leads to an unsustainable loss of quality; thus, other means of recycling are [...] Read more.
Polyethylene terephthalate (PET) is the most widely used polyester plastic, with applications in the textile and packaging industry. Currently, re-moulding is the main path for PET recycling, but this eventually leads to an unsustainable loss of quality; thus, other means of recycling are required. Enzymatic hydrolysis offers the possibility of monomer formation under mild conditions and opens up alternative and infinite recycling paths. Here, IsPETase, derived from the bacterium Ideonella sakaiensis, is considered to be the most active enzyme for PET degradation under mild conditions, and although several studies have demonstrated improvements to both the stability and activity of this enzyme, stability at even moderate temperatures is still an issue. In the present study, we have used sequence and structure-based bioinformatic tools to identify mutations to increase the thermal stability of the enzyme so as to increase PET degradation activity during extended hydrolysis reactions. We found that amino acid substitution S136E showed significant increases to activity and stability. S136E is a previously unreported variant that led to a 3.3-fold increase in activity relative to wild type. Full article
(This article belongs to the Special Issue Advances in Biodegradation of Plastics)
Show Figures

Graphical abstract

12 pages, 977 KiB  
Article
Assessing the Economic Viability of the Plastic Biorefinery Concept and Its Contribution to a More Circular Plastic Sector
by Megan Roux and Cristiano Varrone
Polymers 2021, 13(22), 3883; https://doi.org/10.3390/polym13223883 - 10 Nov 2021
Cited by 13 | Viewed by 3409
Abstract
It is widely accepted that plastic waste is one of the most urgent environmental concerns the world is currently facing. The emergence of bio-based plastics provides an opportunity to reduce dependency on fossil fuels and transition to a more circular plastics economy. For [...] Read more.
It is widely accepted that plastic waste is one of the most urgent environmental concerns the world is currently facing. The emergence of bio-based plastics provides an opportunity to reduce dependency on fossil fuels and transition to a more circular plastics economy. For polyethylene terephthalate (PET), one of the most prevalent plastics in packaging and textiles, two bio-based alternatives exist that are similar or superior in terms of material properties and recyclability. These are polyethylene furanoate (PEF) and polytrimethylene terephthalate (PTT). The overarching aim of this study was to examine the transition from fossil-based to renewable plastics, through the lens of PET upcycling into PEF and PTT. The process for the production of PEF and PTT from three waste feed streams was developed in the SuperPro Designer software and the economic viability assessed via a discounted cumulative cash flow (DCCF) analysis. A techno-economic analysis of the designed process revealed that the minimum selling price (MSP) of second generation-derived PEF and PTT is 3.13 USD/kg, and that utilities and the feedstock used for the production of 2,5-furandicarboxylic acid (FDCA) needed in PEF synthesis contributed the most to the process operating costs. The effect of recycling PEF and PTT through the process at three recycling rates (42%, 50% and 55%) was investigated and it was revealed that increased recycling could reduce the MSP of the 2G bio-plastics (by 48.5%) to 1.61 USD/kg. This demonstrates that the plastic biorefinery, together with increasing recycling rates, would have a beneficial effect on the economic viability of upcycled plastics. Full article
(This article belongs to the Special Issue Advances in Biodegradation of Plastics)
Show Figures

Graphical abstract

14 pages, 2134 KiB  
Article
Quantum Mechanical Investigation of the Oxidative Cleavage of the C–C Backbone Bonds in Polyethylene Model Molecules
by Qixuan Jiang, Zhongyu Li, Ziheng Cui, Ren Wei, Kaili Nie, Haijun Xu and Luo Liu
Polymers 2021, 13(16), 2730; https://doi.org/10.3390/polym13162730 - 15 Aug 2021
Cited by 9 | Viewed by 2939
Abstract
Recalcitrant plastic waste has caused serious global ecological problems. There is an urgent need to develop environmentally friendly and efficient methods for degrading the highly stable carbon skeleton structure of plastics. To that end, we used a quantum mechanical calculation to thoroughly investigate [...] Read more.
Recalcitrant plastic waste has caused serious global ecological problems. There is an urgent need to develop environmentally friendly and efficient methods for degrading the highly stable carbon skeleton structure of plastics. To that end, we used a quantum mechanical calculation to thoroughly investigate the oxidative scission of the carbon-carbon (C–C) backbone in polyethylene (PE). Here, we studied the reaction path of C–C bond oxidation via hydroxyl radical in PE. The flexible force constants and fuzzy bond orders of the C–C bonds were calculated in the presence of one or more carbocations in the same PE carbon chain. By comparison, the strength of the C–C bond decreased when carbocation density increased. However, the higher the density of carbocations, the higher the total energy of the molecule and the more difficult it was to be generated. The results revealed that PE oxidized to alcohol and other products, such as carboxylic acid, aldehyde and ketone, etc. Moreover, the presence of carbocations was seen to promote the cleavage of C–C backbones in the absence of oxygen. Full article
(This article belongs to the Special Issue Advances in Biodegradation of Plastics)
Show Figures

Figure 1

Review

Jump to: Research

23 pages, 4811 KiB  
Review
Towards Sustainable Recycling of Epoxy-Based Polymers: Approaches and Challenges of Epoxy Biodegradation
by Leon Klose, Neele Meyer-Heydecke, Sasipa Wongwattanarat, Jennifer Chow, Pablo Pérez García, Camille Carré, Wolfgang Streit, Garabed Antranikian, Ana Malvis Romero and Andreas Liese
Polymers 2023, 15(12), 2653; https://doi.org/10.3390/polym15122653 - 12 Jun 2023
Cited by 6 | Viewed by 3144
Abstract
Epoxy resins are highly valued for their remarkable mechanical and chemical properties and are extensively used in various applications such as coatings, adhesives, and fiber-reinforced composites in lightweight construction. Composites are especially important for the development and implementation of sustainable technologies such as [...] Read more.
Epoxy resins are highly valued for their remarkable mechanical and chemical properties and are extensively used in various applications such as coatings, adhesives, and fiber-reinforced composites in lightweight construction. Composites are especially important for the development and implementation of sustainable technologies such as wind power, energy-efficient aircrafts, and electric cars. Despite their advantages, their non-biodegradability raises challenges for the recycling of polymer and composites in particular. Conventional methods employed for epoxy recycling are characterized by their high energy consumption and the utilization of toxic chemicals, rendering them rather unsustainable. Recent progress has been made in the field of plastic biodegradation, which is considered more sustainable than energy-intensive mechanical or thermal recycling methods. However, the current successful approaches in plastic biodegradation are predominantly focused on polyester-based polymers, leaving more recalcitrant plastics underrepresented in this area of research. Epoxy polymers, characterized by their strong cross-linking and predominantly ether-based backbone, exhibit a highly rigid and durable structure, placing them within this category. Therefore, the objective of this review paper is to examine the various approaches that have been employed for the biodegradation of epoxy so far. Additionally, the paper sheds light on the analytical techniques utilized in the development of these recycling methods. Moreover, the review addresses the challenges and opportunities entailed in epoxy recycling through bio-based approaches. Full article
(This article belongs to the Special Issue Advances in Biodegradation of Plastics)
Show Figures

Graphical abstract

30 pages, 1864 KiB  
Review
Critical Review on the Progress of Plastic Bioupcycling Technology as a Potential Solution for Sustainable Plastic Waste Management
by Passanun Lomwongsopon and Cristiano Varrone
Polymers 2022, 14(22), 4996; https://doi.org/10.3390/polym14224996 - 18 Nov 2022
Cited by 9 | Viewed by 5328
Abstract
Plastic production worldwide has doubled in the last two decades and is expected to reach a four-fold increase by 2050. The durability of plastic makes them a perfect material for many applications, but it is also a key limitation to their end-of-life management. [...] Read more.
Plastic production worldwide has doubled in the last two decades and is expected to reach a four-fold increase by 2050. The durability of plastic makes them a perfect material for many applications, but it is also a key limitation to their end-of-life management. The current plastic lifecycle is far from circular, with only 13% being collected for recycling and 9% being successfully recycled, indicating the failure of current recycling technology. The remaining plastic waste streams are thus incinerated, landfilled, or worse, mismanaged, leading to them leaking into the environment. To promote plastic circularity, keeping material in the loop is a priority and represents a more sustainable solution. This can be achieved through the reuse of plastic items, or by using plastic waste as a resource for new materials, instead of discarding them as waste. As the discovery of plastic-degrading/utilizing microorganisms and enzymes has been extensively reported recently, the possibility of developing biological plastic upcycling processes is opening up. An increasing amount of studies have investigated the use of plastic as a carbon source for biotechnological processes to produce high-value compounds such as bioplastics, biochemicals, and biosurfactants. In the current review, the advancements in fossil-based plastic bio- and thermochemical upcycling technologies are presented and critically discussed. In particular, we highlight the developed (bio)depolymerization coupled with bioconversion/fermentation processes to obtain industrially valuable products. This review is expected to contribute to the future development and scale-up of effective plastic bioupcycling processes that can act as a drive to increase waste removal from the environment and valorize post-consumer plastic streams, thus accelerating the implementation of a circular (plastic) economy. Full article
(This article belongs to the Special Issue Advances in Biodegradation of Plastics)
Show Figures

Graphical abstract

22 pages, 6119 KiB  
Review
Azelaic Acid: A Bio-Based Building Block for Biodegradable Polymers
by Anamaria Todea, Caterina Deganutti, Mariachiara Spennato, Fioretta Asaro, Guglielmo Zingone, Tiziana Milizia and Lucia Gardossi
Polymers 2021, 13(23), 4091; https://doi.org/10.3390/polym13234091 - 24 Nov 2021
Cited by 11 | Viewed by 5104
Abstract
Azelaic acid is a dicarboxylic acid containing nine C atoms, industrially obtained from oleic acid. Besides its important properties and pharmacological applications, as an individual compound, azelaic acid has proved to be a valuable bio-based monomer for the synthesis of biodegradable and sustainable [...] Read more.
Azelaic acid is a dicarboxylic acid containing nine C atoms, industrially obtained from oleic acid. Besides its important properties and pharmacological applications, as an individual compound, azelaic acid has proved to be a valuable bio-based monomer for the synthesis of biodegradable and sustainable polymers, plasticizers and lubricants. This review discusses the studies and the state of the art in the field of the production of azelaic acid from oleic acid, the chemical and enzymatic synthesis of bio-based oligo and polyester and their properties, including biodegradability and biocompostability. Full article
(This article belongs to the Special Issue Advances in Biodegradation of Plastics)
Show Figures

Figure 1

25 pages, 1792 KiB  
Review
Advantages and Disadvantages of Bioplastics Production from Starch and Lignocellulosic Components
by Mateus Manabu Abe, Júlia Ribeiro Martins, Paula Bertolino Sanvezzo, João Vitor Macedo, Marcia Cristina Branciforti, Peter Halley, Vagner Roberto Botaro and Michel Brienzo
Polymers 2021, 13(15), 2484; https://doi.org/10.3390/polym13152484 - 28 Jul 2021
Cited by 86 | Viewed by 21224
Abstract
The accumulation of plastic wastes in different environments has become a topic of major concern over the past decades; therefore, technologies and strategies aimed at mitigating the environmental impacts of petroleum products have gained worldwide relevance. In this scenario, the production of bioplastics [...] Read more.
The accumulation of plastic wastes in different environments has become a topic of major concern over the past decades; therefore, technologies and strategies aimed at mitigating the environmental impacts of petroleum products have gained worldwide relevance. In this scenario, the production of bioplastics mainly from polysaccharides such as starch is a growing strategy and a field of intense research. The use of plasticizers, the preparation of blends, and the reinforcement of bioplastics with lignocellulosic components have shown promising and environmentally safe alternatives for overcoming the limitations of bioplastics, mainly due to the availability, biodegradability, and biocompatibility of such resources. This review addresses the production of bioplastics composed of polysaccharides from plant biomass and its advantages and disadvantages. Full article
(This article belongs to the Special Issue Advances in Biodegradation of Plastics)
Show Figures

Figure 1

Back to TopTop