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Polymers
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Green Chemistry in Polymer Science and Sustainable Polymers
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Green Chemistry in Polymer Science and Sustainable Polymers

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 December 2021) | Viewed by 38692

Special Issue Editors

Prof. Dr. Nicolas Sbirrazzuoli

E-Mail Website
Guest Editor
Institut de Chimie de Nice UMR CNRS 7272, Université Côte d’Azur, Parc Valrose, 06108 Nice cedex 2, France
Interests: synthetic and bio-based polymers; valorization of second generation biomass and of co-products from industry and bioraffineries; macromolecular chemistry; crystallization kinetics; polymerization kinetics and mechanisms; glass transition; nanostructured materials; nanocomposites; calorimetry; thermal and mechanical properties; rheology; advanced isoconversional methods; circular ecomomy
Dr. Andreia F. Sousa

E-Mail Website
Guest Editor
CICECO and Department of Chemistry, University of Aveiro, 3810-193 Aveiro, Portugal
Interests: polyester synthesis; bio-based materials; recycling; nanocomposite foams
Special Issues, Collections and Topics in MDPI journals
Dr. Nathanael Guigo

E-Mail Website
Guest Editor
Institut de Chimie de Nice UMR CNRS 7272, Université Côte d’Azur, Parc Valrose, 06108 Nice CEDEX 2, France
Interests: structure/property or reactivity/property relations in biopolymers (cellulose, lignins, humins, starch, gelatin) or biobased polymers (polyfurfuryl alcohol, PEF, PBS); furan dicarboxylic acid based polyesters or furanic thermosets based on furfuryl alcohol polycondensation; preparation and characterization of biobased composites and nanocomposites (natural fibres, nanocellulose, nanoclays, graphene, etc.); quiescent crystallization, nucleation, gelation, molecular mobility (glass and sub-glass transitions); thermal degradation; wood modification

Special Issue Information

Dear Colleagues,

Chemistry plays and has played an essential role in the development of modern societies and must therefore constantly adapt in order to contribute to societal progress while respecting ever more stringent health and environmental protection requirements. Unfortunately, the replacement of controversial substances is not always technically possible, nor economically viable. Polymers are no exception to this rule. Despite the countless benefits they bring, scientists must now find solutions to produce polymers that are more respectful of the environment, do not contribute to the depletion of fossil resources, avoid the use of toxic compounds, and whose end of life must be considered. This explains the increasing amount of research in the field of biobased, biodegradable, recyclable, re-shapable, and greener polymers. Thus, chemistry and the field of polymers are fully engaged in the process of transitioning to a greener, carbon-free, more responsible, and circular economy. The aim of this Special Issue is to present a wide overview of scientific papers relating recent advances in the field of “Green Chemistry in Polymer Science and Sustainable Polymers” and will highlight how the use of biomass transformed in biorefineries and co-products from industry can offer realistic solutions to these new challenges for the 21st century. This Special Issue will consider papers dealing with the following aspects:

  • Preparation of biobased monomers from various sources of biomass;
  • Green synthesis of polymers by employing catalysis or enzymatic processes;
  • Characterization and properties of sustainable polymers vs. implemented ones;
  • Life and end-of-life perspectives.

Transversal aspects regarding tecno-economic assessment, life cycle assessment, eco-toxicity, chemical risks, etc. are also warmly encouraged.

Prof. Dr. Nicolas Sbirrazzuoli
Dr. Andreia Sousa
Dr. Nathanael Guigo
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

  • green synthesis
  • biobased polymers
  • biodegradable polymers
  • polymer recycling
  • circular economy

Published Papers (11 papers)

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Research

Jump to: Review

12 pages, 2914 KiB  
Article
Furanic Humins from Biorefinery as Biobased Binder for Bitumen
by Anna Sangregorio, Nathanael Guigo, Luc Vincent, Ed de Jong and Nicolas Sbirrazzuoli
Polymers 2022, 14(5), 1019; https://doi.org/10.3390/polym14051019 - 3 Mar 2022
Cited by 3 | Viewed by 1879
Abstract
To decrease the environmental impact of bitumen, more sustainable binders should be proposed. This study emphasizes how industrial humins co-produced during the biorefining of carbohydrates can be employed as a macromolecular binder for bitumen. Humins are heterogeneous polyfuranic compounds, and they were mixed [...] Read more.
To decrease the environmental impact of bitumen, more sustainable binders should be proposed. This study emphasizes how industrial humins co-produced during the biorefining of carbohydrates can be employed as a macromolecular binder for bitumen. Humins are heterogeneous polyfuranic compounds, and they were mixed at 50 wt% with bitumen. When the non-water-soluble fractions of humins were employed (Hns), no variation of the chemical structure was observed in FTIR spectra after the mixing. The DSC investigations showed that the crystallization of aromatic fractions in bitumen shifted to higher temperature for humins’ modified bitumen. The thermogravimetric data highlighted that the presence of humins or Hns in bitumen can lead to mass loss below 200 °C. The rheological investigations highlighted some key advantages of using humins or Hns with bitumen. At high temperatures, the storage modulus of the modified bitumen is increased and shows lower susceptibility to variations in frequency. At low temperatures, the phase angle of Hns-modified bitumen is lower than that of bitumen, suggesting less temperature susceptibility as a consequence of a cross-linked network formation. Full article
(This article belongs to the Special Issue Green Chemistry in Polymer Science and Sustainable Polymers)
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16 pages, 3379 KiB  
Article
Synthesis of Biobased and Hybrid Polyurethane Xerogels from Bacterial Polyester for Potential Biomedical Applications
by Sophie Wendels, Deyvid de Souza Porto and Luc Avérous
Polymers 2021, 13(23), 4256; https://doi.org/10.3390/polym13234256 - 4 Dec 2021
Cited by 6 | Viewed by 1723
Abstract
Organic–inorganic xerogel networks were synthesized from bacterial poly (3-hydroxybutyrate) (PHB) for potential biomedical applications. Since silane-based networks usually demonstrate increased biocompatibility and mechanical properties, siloxane groups have been added onto polyurethane (PU) architectures. In this work, a diol oligomer (oligoPHB-diol) was first prepared [...] Read more.
Organic–inorganic xerogel networks were synthesized from bacterial poly (3-hydroxybutyrate) (PHB) for potential biomedical applications. Since silane-based networks usually demonstrate increased biocompatibility and mechanical properties, siloxane groups have been added onto polyurethane (PU) architectures. In this work, a diol oligomer (oligoPHB-diol) was first prepared from bacterial poly(3-hydroxybutyrate) (PHB) with an environmentally friendly method. Then, hexamethylene diisocyanate or biobased dimeryl diisocyanate was used as diisocyanate to react with the short oligoPHB-diol for the synthesis of different NCO-terminated PU systems in a bulk process and without catalyst. Various PU systems containing increasing NCO/OH molar ratios were prepared. Siloxane precursors were then obtained after reaction of the NCO-terminated PUs with (3-aminopropyl)triethoxysilane, resulting in silane-terminated polymers. These structures were confirmed by different analytical techniques. Finally, four series of xerogels were prepared via a sol–gel process from the siloxane precursors, and their properties were evaluated depending on varying parameters such as the inorganic network crosslinking density. The final xerogels exhibited adequate properties in connection with biomedical applications such as a high in vitro degradation up to 15 wt% after 12 weeks. Full article
(This article belongs to the Special Issue Green Chemistry in Polymer Science and Sustainable Polymers)
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17 pages, 4116 KiB  
Article
Ferulic Acid as Building Block for the Lipase-Catalyzed Synthesis of Biobased Aromatic Polyesters
by Alfred Bazin, Luc Avérous and Eric Pollet
Polymers 2021, 13(21), 3693; https://doi.org/10.3390/polym13213693 - 27 Oct 2021
Cited by 8 | Viewed by 2228
Abstract
Enzymatic synthesis of aromatic biobased polyesters is a recent and rapidly expanding research field. However, the direct lipase-catalyzed synthesis of polyesters from ferulic acid has not yet been reported. In this work, various ferulic-based monomers were considered for their capability to undergo CALB-catalyzed [...] Read more.
Enzymatic synthesis of aromatic biobased polyesters is a recent and rapidly expanding research field. However, the direct lipase-catalyzed synthesis of polyesters from ferulic acid has not yet been reported. In this work, various ferulic-based monomers were considered for their capability to undergo CALB-catalyzed polymerization. After conversion into diesters of different lengths, the CALB-catalyzed polymerization of these monomers with 1,4-butanediol resulted in short oligomers with a DPn up to 5. Hydrogenation of the double bond resulted in monomers allowing obtaining polyesters of higher molar masses with DPn up to 58 and Mw up to 33,100 g·mol−1. These polyesters presented good thermal resistance up to 350 °C and Tg up to 7 °C. Reduction of the ferulic-based diesters into diols allowed preserving the double bond and synthesizing polyesters with a DPn up to 19 and Mw up to 15,500 g·mol−1 and higher Tg (up to 21 °C). Thus, this study has shown that the monomer hydrogenation strategy proved to be the most promising route to achieve ferulic-based polyester chains of high DPn. This study also demonstrates for the first time that ferulic-based diols allow the synthesis of high Tg polyesters. Therefore, this is an important first step toward the synthesis of competitive biobased aromatic polyesters by enzymatic catalysis. Full article
(This article belongs to the Special Issue Green Chemistry in Polymer Science and Sustainable Polymers)
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17 pages, 9101 KiB  
Article
Comparative Analysis of the Mechanical Behaviour of PEF and PET Uniaxial Stretching Based on the Time/Temperature Superposition Principle
by Emilie Forestier, Christelle Combeaud, Nathanael Guigo, Guillaume Corvec, Christophe Pradille, Nicolas Sbirrazzuoli and Noelle Billon
Polymers 2021, 13(19), 3295; https://doi.org/10.3390/polym13193295 - 27 Sep 2021
Cited by 14 | Viewed by 2772
Abstract
Poly(ethylene 2,5-furandicarboxylate), PEF and poly(ethylene terephthalate), PET, are two polyesters with close chemical structures. It leads to similar thermal, mechanical and barrier properties. In order to optimize their stretching, a strategy based on the time/temperature principle is used. The building of master curves, [...] Read more.
Poly(ethylene 2,5-furandicarboxylate), PEF and poly(ethylene terephthalate), PET, are two polyesters with close chemical structures. It leads to similar thermal, mechanical and barrier properties. In order to optimize their stretching, a strategy based on the time/temperature principle is used. The building of master curves, in the linear visco-elastic domain, allows the identification of the experimental conditions for which the two materials are in the same physical state. The initial physical state of the materials is important as, to fit with the industrial constrains, the polymers must reach high level of deformation, and develop strain induced crystallization (SIC). In this paper, the screening of the forming range is described, as well as the mechanical response depending on the stretching settings. Moreover, the same mechanical response can exist for PEF and PET if the same gap from the α-relaxation exists. Full article
(This article belongs to the Special Issue Green Chemistry in Polymer Science and Sustainable Polymers)
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18 pages, 4287 KiB  
Article
Influence of Reactive Chain Extension on the Properties of 3D Printed Poly(Lactic Acid) Constructs
by Maria-Eirini Grigora, Zoi Terzopoulou, Konstantinos Tsongas, Panagiotis Klonos, Nikolaos Kalafatakis, Dimitrios N. Bikiaris, Apostolos Kyritsis and Dimitrios Tzetzis
Polymers 2021, 13(9), 1381; https://doi.org/10.3390/polym13091381 - 23 Apr 2021
Cited by 27 | Viewed by 3292
Abstract
Fused deposition modeling (FDM) is currently the most popular 3D printing method, where thermoplastic polymers are predominantly used. Among them, the biobased poly(lactic acid) (PLA) governs the FDM filament market, with demand higher than supply, since not all grades of PLA are suitable [...] Read more.
Fused deposition modeling (FDM) is currently the most popular 3D printing method, where thermoplastic polymers are predominantly used. Among them, the biobased poly(lactic acid) (PLA) governs the FDM filament market, with demand higher than supply, since not all grades of PLA are suitable for FDM filament production. In this work, the effect of a food grade chain extender (Joncryl ADR® 4400) on the physicochemical properties and printability of PLA marketed for injection molding was examined. All samples were characterized in terms of their mechanical and thermal properties. The microstructure of the filaments and 3D-printed fractured surfaces following tensile testing were examined with optical and scanning electron microscopy, respectively. Molecular weight and complex viscosity increased, while the melt flow index decreased after the incorporation of Joncryl, which resulted in filaments of improved quality and 3D-printed constructs with enhanced mechanical properties. Dielectric spectroscopy revealed that the bulk properties of PLA with respect to molecular mobility, both local and segmental, were, interestingly, not affected by the modifier. Indirectly, this may suggest that the major effects of the extender are on chain length, without inducing chain branching, at least not to a significant extent. Full article
(This article belongs to the Special Issue Green Chemistry in Polymer Science and Sustainable Polymers)
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20 pages, 2237 KiB  
Article
Fully Bio-Based Thermosetting Polyurethanes from Bio-Based Polyols and Isocyanates
by Roberto Morales-Cerrada, Romain Tavernier and Sylvain Caillol
Polymers 2021, 13(8), 1255; https://doi.org/10.3390/polym13081255 - 13 Apr 2021
Cited by 55 | Viewed by 7816
Abstract
The trend towards the utilization of bioresources for the manufacturing of polymers has led industry players to bring to the market new monomers. In this work, we studied 3 polyisocyanates and 2 polyols with high renewable carbon contents, namely L-lysine ethyl ester diisocyanate [...] Read more.
The trend towards the utilization of bioresources for the manufacturing of polymers has led industry players to bring to the market new monomers. In this work, we studied 3 polyisocyanates and 2 polyols with high renewable carbon contents, namely L-lysine ethyl ester diisocyanate (LDI), pentamethylene-diisocyanate (PDI) isocyanurate trimer, and hexamethylene-diisocyanate (HDI) allophanate as the isocyanates, as well as castor oil and polypropanediol as the polyols. These monomers are commercially available at a large scale and were used in direct formulations or used as prepolymers. Thermosetting polymers with Tg values ranging from −41 to +21 °C and thermal stabilities of up to 300 °C were obtained, and the polymerization was studied using NMR, DSC, and rheology. Cured materials were also characterized using FTIR, DMA, gel content, and swelling index determinations. These high bio-based content materials can successfully be obtained and could be used as alternatives to petro-based materials. Full article
(This article belongs to the Special Issue Green Chemistry in Polymer Science and Sustainable Polymers)
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23 pages, 6770 KiB  
Article
The Effect of Surface Treatment with Isocyanate and Aromatic Carbodiimide of Thermally Expanded Vermiculite Used as a Functional Filler for Polylactide-Based Composites
by Mateusz Barczewski, Olga Mysiukiewicz, Aleksander Hejna, Radosław Biskup, Joanna Szulc, Sławomir Michałowski, Adam Piasecki and Arkadiusz Kloziński
Polymers 2021, 13(6), 890; https://doi.org/10.3390/polym13060890 - 14 Mar 2021
Cited by 19 | Viewed by 3318
Abstract
In this work, thermally expanded vermiculite (TE-VMT) was surface modified and used as a filler for composites with a polylactide (PLA) matrix. Modification of vermiculite was realized by simultaneous ball milling with the presence of two PLA chain extenders, aromatic carbodiimide (KI), and [...] Read more.
In this work, thermally expanded vermiculite (TE-VMT) was surface modified and used as a filler for composites with a polylactide (PLA) matrix. Modification of vermiculite was realized by simultaneous ball milling with the presence of two PLA chain extenders, aromatic carbodiimide (KI), and 4,4’-methylenebis(phenyl isocyanate) (MDI). In addition to analyzing the particle size of the filler subjected to processing, the efficiency of mechanochemical modification was evaluated by Fourier transform infrared spectroscopy (FTIR) and scanning electron microscopy (SEM). The composites of PLA with three vermiculite types were prepared by melt mixing and subjected to mechanical, thermomechanical, thermal, and structural evaluation. The structure of composites containing a constant amount of the filler (20 wt%) was assessed using FTIR spectroscopy and SEM analysis supplemented by evaluating the final injection-molded samples’ physicochemical properties. Mechanical behavior of the composites was assessed by static tensile test and impact strength hardness measurements. Heat deflection temperature (HDT) test and dynamic thermomechanical analysis (DMTA) were applied to evaluate the influence of the filler addition and its functionalization on thermomechanical properties of PLA-based composites. Thermal properties were assessed by differential scanning calorimetry (DSC), pyrolysis combustion flow calorimetry (PCFC), and thermogravimetric analysis (TGA). The use of filler-reactive chain extenders (CE) made it possible to change the vermiculite structure and obtain an improvement in interfacial adhesion and more favorable filler dispersions in the matrix. This translated into an improvement in impact strength and an increase in thermo-mechanical stability and heat release capacity of composites containing modified vermiculites. Full article
(This article belongs to the Special Issue Green Chemistry in Polymer Science and Sustainable Polymers)
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15 pages, 5491 KiB  
Article
Electrochemical Activity of Lignin Based Composite Membranes
by Marya Baloch, Mikel Alberro and Jalel Labidi
Polymers 2021, 13(4), 643; https://doi.org/10.3390/polym13040643 - 21 Feb 2021
Cited by 8 | Viewed by 2759
Abstract
Our society’s most pressing challenges, like high CO2 emission and the constant battle against energy poverty, require a clean and easier solution to store and utilize the renewable energy resources. However, recent electrochemical components are expensive and harmful to the environment, which [...] Read more.
Our society’s most pressing challenges, like high CO2 emission and the constant battle against energy poverty, require a clean and easier solution to store and utilize the renewable energy resources. However, recent electrochemical components are expensive and harmful to the environment, which restricts their widespread deployment. This study proposes an easy method to synthesize and fabricate composite membranes with abundantly found biomass lignin polymer to replace conventional costly and toxic electrode materials. Easier manipulation of lignin within the polymeric matrix could provide the improved composite to enhance its electrochemical activity. Our major focus is to activate the quinone moiety via oxidation in the polymeric mixture using a strong ionic acid. The physico-chemical and electrochemical characterizations of two different lignins within varied polymeric mixture compositions have been carried out to confirm that the redox properties of pure unmodified lignin could be achieved via intrinsic mutual sharing of the structural properties and intercross linkage leading to improved integrity and redox activity/conductivity. Full article
(This article belongs to the Special Issue Green Chemistry in Polymer Science and Sustainable Polymers)
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13 pages, 14811 KiB  
Article
Non-Furanic Humins-Based Non-Isocyanate Polyurethane (NIPU) Thermoset Wood Adhesives
by Xinyi Chen, Antonio Pizzi, Hisham Essawy, Emmanuel Fredon, Christine Gerardin, Nathanael Guigo and Nicolas Sbirrazzuoli
Polymers 2021, 13(3), 372; https://doi.org/10.3390/polym13030372 - 25 Jan 2021
Cited by 16 | Viewed by 3119
Abstract
Predominantly non-furanic commercial humins were used to prepare humin-based non-isocyanate polyurethane (NIPU) resins for wood panel adhesives. Pure humin-based NIPU resins and tannin–humin NIPU resins were prepared, the latter to upgrade the humins’ performance. Species in the raw humins and species formed in [...] Read more.
Predominantly non-furanic commercial humins were used to prepare humin-based non-isocyanate polyurethane (NIPU) resins for wood panel adhesives. Pure humin-based NIPU resins and tannin–humin NIPU resins were prepared, the latter to upgrade the humins’ performance. Species in the raw humins and species formed in the NIPU resins were identified by Matrix Assisted Laser Desorption Ionization Time of Flight (MALDI ToF) spectrometry and Fourier Transform Infrared (FTIR). Humins, fulvic acid and derivatives, humic acid and its fragments, some lignans present and furanic oligomers present formed NIPU linkages. Thermomechanical analysis (TMA) showed that as with other biomaterials-based NIPU resins, all these resins also showed two temperature peaks of curing, the first around 130 °C and the second around 220 °C. A decrease in the Modulus of Elasticity (MOE) between the two indicated that the first curing period corresponded to linear growth of the oligomers forming a physical entanglement network. This then disentangled, and the second corresponded to the formation of a chemical cross-linked network. This second peak was more evident for the tannin–humin NIPU resins. All the laboratory particleboard made and tested either bonded with pure humins or with tannin–humin NIPU adhesives satisfied well the internal bond strength requirements of the relevant standard for interior grade panels. The tannin–humin adhesives performed clearly better than the pure humins one. Full article
(This article belongs to the Special Issue Green Chemistry in Polymer Science and Sustainable Polymers)
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Review

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30 pages, 7215 KiB  
Review
Green Aspects in Molecularly Imprinted Polymers by Biomass Waste Utilization
by Roberta Del Sole, Giuseppe Mele, Ermelinda Bloise and Lucia Mergola
Polymers 2021, 13(15), 2430; https://doi.org/10.3390/polym13152430 - 23 Jul 2021
Cited by 28 | Viewed by 3994
Abstract
Molecular Imprinting Polymer (MIP) technology is a technique to design artificial receptors with a predetermined selectivity and specificity for a given analyte, which can be used as ideal materials in various application fields. In the last decades, MIP technology has gained much attention [...] Read more.
Molecular Imprinting Polymer (MIP) technology is a technique to design artificial receptors with a predetermined selectivity and specificity for a given analyte, which can be used as ideal materials in various application fields. In the last decades, MIP technology has gained much attention from the scientific world as summarized in several reviews with this topic. Furthermore, green synthesis in chemistry is nowadays one of the essential aspects to be taken into consideration in the development of novel products. In accordance with this feature, the MIP community more recently devoted considerable research and development efforts on eco-friendly processes. Among other materials, biomass waste, which is a big environmental problem because most of it is discarded, can represent a potential sustainable alternative source in green synthesis, which can be addressed to the production of high-value carbon-based materials with different applications. This review aims to focus and explore in detail the recent progress in the use of biomass waste for imprinted polymers preparation. Specifically, different types of biomass waste in MIP preparation will be exploited: chitosan, cellulose, activated carbon, carbon dots, cyclodextrins, and waste extracts, describing the approaches used in the synthesis of MIPs combined with biomass waste derivatives. Full article
(This article belongs to the Special Issue Green Chemistry in Polymer Science and Sustainable Polymers)
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16 pages, 1020 KiB  
Review
Recent Advances in Renewable Polymer Production from Lignin-Derived Aldehydes
by Nahyeon Lee, Yong Tae Kim and Jechan Lee
Polymers 2021, 13(3), 364; https://doi.org/10.3390/polym13030364 - 24 Jan 2021
Cited by 12 | Viewed by 3628
Abstract
Lignin directly derived from lignocellulosic biomass has been named a promising source of platform chemicals for the production of bio-based polymers. This review discusses potentially relevant routes to produce renewable aromatic aldehydes (e.g., syringaldehyde and vanillin) from lignin feedstocks (pre-isolated lignin or lignocellulose) [...] Read more.
Lignin directly derived from lignocellulosic biomass has been named a promising source of platform chemicals for the production of bio-based polymers. This review discusses potentially relevant routes to produce renewable aromatic aldehydes (e.g., syringaldehyde and vanillin) from lignin feedstocks (pre-isolated lignin or lignocellulose) that are used to synthesize a range of bio-based polymers. To do this, the processes to make aromatic aldehydes from lignin with their highest available yields are first presented. After that, the routes from such aldehydes to different polymers are explored. Challenges and perspectives of the production the lignin-derived renewable chemicals and polymers are also highlighted. Full article
(This article belongs to the Special Issue Green Chemistry in Polymer Science and Sustainable Polymers)
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