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Green Polymeric Materials and Sustainable Valorization of Natural Resources

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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 (31 October 2021) | Viewed by 28674

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Special Issue Editors

Prof. Dr. George Z. Papageorgiou

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Guest Editor

1. Department of Chemistry, University of Ioannina, P.O. Box 1186, GR-45110 Ioannina, Greece
2. Institute of Materials Science and Computing, University Research Center of Ioannina (URCI), 45110 Ioannina, Greece
Interests: sustainable and green industrial chemistry; polymer nanocomposites; materials characterization
Special Issues, Collections and Topics in MDPI journals

Dr. Dimitrios G. Papageorgiou

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Guest Editor

School of Engineering and Materials Science, Queen Mary University of London, Mile End Road, London E1 4NS, UK
Interests: polymer nanocomposites; nanomaterials; graphene; 2D materials; nanocarbons; strain engineering; raman spectroscopy; micromechanics; polymer engineering; bio-based polymers and composites
Special Issues, Collections and Topics in MDPI journals

Special Issue Information

Dear Colleagues,

The application of Green Chemistry concept in industrial chemistry, and particularly in the production and use of polymeric materials aims at reducing the manipulation and formation of hazardous substances during their production and life cycle. The above goals are usually achieved with the use of renewable raw materials and eco-friendly solvents, along with “green” product design and impact including safety, sustainability, degradation and recyclability. Furthermore, benign synthesis and catalysis, solvent-free processes, process design and intensification, as well as energy use issues are of crucial importance in the manufacturing of green and sustainable polymeric materials.

Over the past few decades, the production and applications of synthetic polymers showed an exponential increase. Recently, concerns regarding depletion of fossil resources, disposal-related issues, as well as government policies, have led to a continuously growing interest in the development of green, sustainable and safe environmentally-friendly plastics from renewable resources.

In general, there are three key approaches towards green plastics. The first approach is associated with the biorefinery concept, applying sustainable processes and using biomass from feedstocks. Renewable polymers are isolated from natural biopolymers or synthesized from biobased monomers. Carbohydrates such as cellulose, lignin, starch, terpenes, proteins, chitosan, and biopolyesters can be chemically modified. In fact, efforts are being made to synthesize traditional monomers and platform chemicals from renewable resources. Thus, ethylene, propylene, as well as butadiene can be produced from bioethanol. Diols, such as ethylene glycol, 1,3-propanediol, 1,4-butanediol, and also polyols, diacids, etc., are also available nowadays. In this way, traditional polymers, such as polyethylene, polypropylene, poly(ethylene terephthalate), or polystyrene, can be now considered biobased. In addition, novel biobased thermoplastic and thermoset polymers have gained increasing interest. Organic acid monomers from renewable resources include glycolic, 3-hydroxypropionic, lactic, succinic, itaconic, muconic, adipic, levulinic, vanillic and 2,5-furandicarboxylic acids, while important alcohol monomers such as isosorbide, xylitol, sorbitol, glycerol can be derived from sugars.

Poly(ethylene 2,5-furandicarboxylate) (PEF) is a typical example of a new recyclable and fully biobased thermoplastic polymer. The industrial production of PEF is associated with reduced non-renewable energy use, low carbon footprint and atom economy. Furthermore, biodegradable polymers, such as poly(hydroxybutyrate) (PHB), poly(lactic acid) (PLA), poly(butylene succinate) (PBS), chitosan and others, are of special importance among sustainable polymers from renewable resources, considering the end of their life cycle.

The biotechnology approach uses living cells to produce biopolymers by essentially converting them into solar power reactors. Recent research efforts have shown that it is possible to create synthetic polymers within living cells, thus opening up a new area of chemical biology.

Finally, green polymers can be produced by activating and polymerizing carbon dioxide. For example, carbon dioxide can react with oxiranes, to produce cyclic carbonates. Eco-friendly materials such as non-isocyanate polyurethanes and polypropylene carbonate can be obtained.

The aim of this Special Issue is to highlight the progress on monomers from biorefinery, synthesis, industrial processes and benign catalysts, characterization, properties, applications, degradation, life cycle assessment, reuse and recycling of green and sustainable polymers, copolymers, blends and composites.

Prof. Dr. George Z. Papageorgiou
Dr. Dimitrios G. Papageorgiou
Guest Editors

Keywords

green chemistry
sustainable materials
natural polymers
biobased polymers
biodegradable polymers
biopolymers
biorefinery
benign catalysts
benign polymer synthesis
renewable resources
biomass
poly(ethylene 2,5-furandicarboxylate)
poly(lactic acid)
chitosan
renewable monomers
2,5-furandicarboxylic acid
lignin
cellulose
polysaccharides
life cycle
degradation
recycling

Published Papers (4 papers)

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Research

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25 pages, 13370 KiB

Open AccessArticle

Biobased Terpene Derivatives: Stiff and Biocompatible Compounds to Tune Biodegradability and Properties of Poly(butylene succinate)

by Reza Zeinali, Luis J. del Valle, Lourdes Franco, Ibraheem Yousef, Jeroen Rintjema, Carlos Alemán, Fernando Bravo, Arjan W. Kleij and Jordi Puiggalí

Polymers 2022, 14(1), 161; https://doi.org/10.3390/polym14010161 - 31 Dec 2021

Cited by 6 | Viewed by 2703

Abstract

Different copolymers incorporating terpene oxide units (e.g., limonene oxide) have been evaluated considering thermal properties, degradability, and biocompatibility. Thus, polycarbonates and polyesters derived from aromatic, monocyclic and bicyclic anhydrides have been considered. Furthermore, ring substitution with myrcene terpene has been evaluated. All polymers were amorphous when evaluated directly from synthesis. However, spherulites could be observed after the slow evaporation of diluted chloroform solutions of polylimonene carbonate, with all isopropene units possessing an R configuration. This feature was surprising considering the reported information that suggested only the racemic polymer was able to crystallize. All polymers were thermally stable and showed a dependence of the maximum degradation rate temperature (from 242 °C to 342 °C) with the type of terpene oxide. The graduation of glass transition temperatures (from 44 °C to 172 °C) was also observed, being higher than those corresponding to the unsubstituted polymers. The chain stiffness of the studied polymers hindered both hydrolytic and enzymatic degradation while a higher rate was detected when an oxidative medium was assayed (e.g., weight losses around 12% after 21 days of exposure). All samples were biocompatible according to the adhesion and proliferation tests performed with fibroblast cells. Hydrophobic and mechanically consistent films (i.e., contact angles between 90° and 110°) were obtained after the evaporation of chloroform from the solutions, having different ratios of the studied biobased polyterpenes and poly(butylene succinate) (PBS). The blend films were comparable in tensile modulus and tensile strength with the pure PBS (e.g., values of 330 MPa and 7 MPa were determined for samples incorporating 30 wt.% of poly(PA-LO), the copolyester derived from limonene oxide and phthalic anhydride. Blends were degradable, biocompatible and appropriate to produce oriented-pore and random-pore scaffolds via a thermally-induced phase separation (TIPS) method and using 1,4-dioxane as solvent. The best results were attained with the blend composed of 70 wt.% PBS and 30 wt.% poly(PA-LO). In summary, the studied biobased terpene derivatives showed promising properties to be used in a blended form for biomedical applications such as scaffolds for tissue engineering. Full article

(This article belongs to the Special Issue Green Polymeric Materials and Sustainable Valorization of Natural Resources)

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12 pages, 2038 KiB

Open AccessArticle

Active Biodegradable Films Based on Sweet Lime Peel Residue and Its Effect on Quality of Fish Fillets

by Yasir Arafat, Ammar Altemimi, Anubhav Pratap-Singh and Laxmikant S. Badwaik

Polymers 2021, 13(8), 1240; https://doi.org/10.3390/polym13081240 - 12 Apr 2021

Cited by 9 | Viewed by 2903

Abstract

Residual sweet lime peels after the extraction of essential oil by solvent free microwave extraction were used for developing biodegradable film. Glycerol as a plasticizer, soya lecithin as an emulsifier and sweet lime essential oil (0, 1, 2 and 3%) as an active agent was employed. Developed films were analyzed for their mechanical, barrier and antimicrobial properties. The films (with 3% essential oil) which reported highest antimicrobial property against E. coli (24.24 ± 2.69 mm) were wrapped on fish fillet and stored at the refrigerated condition for 12 days. The quality of fish fillets was evaluated every 4 days and compared with polyethylene wrapped and control fish fillets. The active film wrapped sample showed less surface microbial count (3.28 ± 0.16 log cfu/cm²) compared to polyethylene wrapped sample. The hardness values were increased during storage and cohesiveness and springiness of all wrapped samples decreased from day 0 to day 12. Full article

(This article belongs to the Special Issue Green Polymeric Materials and Sustainable Valorization of Natural Resources)

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19 pages, 4341 KiB

Open AccessArticle

A New Era in Engineering Plastics: Compatibility and Perspectives of Sustainable Alipharomatic Poly(ethylene terephthalate)/Poly(ethylene 2,5-furandicarboxylate) Blends

by Dimitrios G. Papageorgiou, Irini Tsetsou, Raphael O. Ioannidis, George N. Nikolaidis, Stylianos Exarhopoulos, Nejib Kasmi, Dimitrios N. Bikiaris, Dimitris S. Achilias and George Z. Papageorgiou

Polymers 2021, 13(7), 1070; https://doi.org/10.3390/polym13071070 - 29 Mar 2021

Cited by 10 | Viewed by 4493

Abstract

The industrialisation of poly(ethylene 2,5-furandicarboxylate) for total replacement of poly(ethylene terephthalate) in the polyester market is under question. Preparation of high-performing polymer blends is a well-established strategy for tuning the properties of certain homopolymers and create tailor-made materials to meet the demands for a number of applications. In this work, the structure, thermal properties and the miscibility of a series of poly(ethylene terephthalate)/poly(ethylene 2,5-furandicarboxylate) (PET/PEF) blends have been studied. A number of thermal treatments were followed in order to examine the thermal transitions, their dynamic state and the miscibility characteristics for each blend composition. Based on their glass transition temperatures and melting behaviour the PET/PEF blends are miscible at high and low poly(ethylene terephthalate) (PET) contents, while partial miscibility was observed at intermediate compositions. The multiple melting was studied and their melting point depression was analysed with the Flory-Huggins theory. In an attempt to further improve miscibility, reactive blending was also investigated. Full article

(This article belongs to the Special Issue Green Polymeric Materials and Sustainable Valorization of Natural Resources)

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Review

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32 pages, 71459 KiB

Open AccessReview

The Road to Bring FDCA and PEF to the Market

by Ed de Jong, Hendrikus (Roy) A. Visser, Ana Sousa Dias, Clare Harvey and Gert-Jan M. Gruter

Polymers 2022, 14(5), 943; https://doi.org/10.3390/polym14050943 - 26 Feb 2022

Cited by 64 | Viewed by 16986

Abstract

Biobased polymers and materials are desperately needed to replace fossil-based materials in the world’s transition to a more sustainable lifestyle. In this article, Avantium describes the path from invention towards commercialization of their YXY^® plants-to-plastics Technology, which catalytically converts plant-based sugars into FDCA—the chemical building block for PEF (polyethylene furanoate). PEF is a plant-based, highly recyclable plastic, with superior performance properties compared to today’s widely used petroleum-based packaging materials. The myriad of topics that must be addressed in the process of bringing a new monomer and polymer to market are discussed, including process development and application development, regulatory requirements, IP protection, commercial partnerships, by-product valorisation, life cycle assessment (LCA), recyclability and circular economy fit, and end-of-life. Advice is provided for others considering embarking on a similar journey, as well as an outlook on the next, exciting steps towards large-scale production of FDCA and PEF at Avantium’s Flagship Plant and beyond. Full article

(This article belongs to the Special Issue Green Polymeric Materials and Sustainable Valorization of Natural Resources)

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