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A special issue of Polymers (ISSN 2073-4360). This special issue belongs to the section "Biomacromolecules, Biobased and Biodegradable Polymers".

Deadline for manuscript submissions: closed (31 August 2022) | Viewed by 32730

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Dr. Raluca Nicoleta Darie-Nita

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Petru Poni Institute of Macromolecular Chemistry, Grigore Ghica Voda Alley 41A, 700487 Iasi, Romania
Interests: reactive processing (natural and synthetic polymers); physico-chemical characterization of polymers and composites (rheological, mechanical, thermal, and surface properties); biodegradable polymers; applications of bio-based materials
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Dr. Maria Râpă

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Faculty of Material Sciences and Engineering, Politehnica University of Bucharest, Bucharest, Romania
Interests: biodegradable polymers; polymer processing technologies; characterization; applications of bio-based materials
Special Issues, Collections and Topics in MDPI journals

Special Issue Information

Dear Colleagues,

Polyesters represent one of the most important classes of polymers with an increased demand on the market. In addition to the well-known polyethylene terephthalate (PET), polybutylene terephthalate (PBT), and polycaprolactone (PCL), which are petroleum-derived polyesters, the versatility of the ester linkage has increased the development of novel biobased polyesters and copolyesters from renewable resources, among them polylactic acid (PLA) and polyhydroxyalkanoates (PHAs) being the most competitive biodegradable polymers commercialized so far. Novel approaches are in a constant drive to develop new sources for biobased polyesters for diverse applications, as well as to improve the properties of known polyesters and their resulting materials.

This Special Issue invites original papers and reviews reporting the most valuable findings on polyester-based materials. Insights into polyester functionalization, copolymerization, surface modification or use of a diversity of additives or fillers in order to widen the development and performance of polyester-based materials in various industries, such as packaging, automotive, constructions, electronics, textile or the medical field, are welcome. Studies regarding the environmental impact and in particular recyclability or (bio)degradation of the polyester-based materials can also be included in this Special Issue.

Dr. Raluca Nicoleta DARIE-NIȚĂ
Dr. Maria RÂPĂ
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

biobased polyesters
synthetic polyesters
additives
bio(degradation)
materials
characterization
applications

Related Special Issue

Polyesters in Polymers (56 articles)

Published Papers (9 papers)

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Research

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19 pages, 5416 KiB

Open AccessArticle

Controlled and Accelerated Hydrolysis of Polylactide (PLA) through Pentaerythritol Phosphites with Acid Scavengers

by Matthias Polidar, Elke Metzsch-Zilligen and Rudolf Pfaendner

Polymers 2022, 14(19), 4237; https://0-doi-org.brum.beds.ac.uk/10.3390/polym14194237 - 10 Oct 2022

Cited by 9 | Viewed by 3209

Abstract

This study provides insight into the accelerated hydrolysis of polyester PLA through the addition of phosphites based on pentaerythritol. To control hydrolysis and ensure processing stability, different types of phosphites and combinations of phosphites with acid scavengers were studied. Therefore, commercially available PLA was compounded with selected additives on a twin-screw extruder, and hydrolysis experiments were performed at 23 °C, 35 °C and 58 °C in deionized water. Hydrolysis of PLA was evaluated by the melt volume rate (MVR) and size-exclusion chromatography (SEC). For example, after 4 days of water storage at 58 °C, the number average molecular weight of the PLA comparison sample was reduced by 31.3%, whereas PLA compounded with 0.8% phosphite P1 had a 57.7% lower molecular weight. The results are in good agreement with the expected and tested stability against hydrolysis of the investigated phosphite structures. ³¹P-NMR spectroscopy was utilized to elucidate the hydrolysis of phosphites in the presence of lactic acid. With the addition of phosphites based on pentaerythritol, the hydrolysis rate can be enhanced, and faster biodegradation behavior of biodegradable polyesters is expected. Accelerated biodegradation is beneficial for reducing the residence time of polymers in composting facilities or during home composting and as litter or microplastic residues. Full article

(This article belongs to the Special Issue Polyester-Based Materials)

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14 pages, 4374 KiB

Open AccessArticle

The Incorporation of Low-Molecular Weight Poly(Mannitol Sebacate)s on PLA Electrospun Fibers: Effects on the Mechanical Properties and Surface Chemistry

by Víctor Hevilla, Águeda Sonseca, Enrique Gimenez, Coro Echeverría, Alexandra Muñoz-Bonilla and Marta Fernández-García

Polymers 2022, 14(16), 3342; https://0-doi-org.brum.beds.ac.uk/10.3390/polym14163342 - 16 Aug 2022

Cited by 2 | Viewed by 1615

Abstract

We offer a report on the synthesis of low-molecular weight biobased poly(mannitol sebacate) (PMS) and its functionalization with acrylate groups (PMSAc). These synthesized polyesters were blended at a low level (10 wt%) with poly (lactic acid) PLA to prepare aligned fibers by electrospinning, coupled with a rotatory collector. The obtained fibers were extensively studied by Fourier transform infrared spectroscopy (FTIR), scanning electron microscopy (SEM), differential scanning calorimetry (DSC), and wide-angle X-ray diffraction (WAXS), employing synchrotron radiation. The incorporation of the PMSs on the PLA fibers did not significantly affect the fiber diameters, whereas the alignment was almost maintained. The crystallinity and thermal properties were also slightly modified with the addition of PMSs, and an increase in the degree of crystallinity and in the glass transition temperature of the blend compared to PLA was observed. Remarkably, the PLA/PMSs fibers were more ductile due to the elastomeric character of PMS, with higher values of elongation at break and tensile strengths, and a smaller Young modulus in comparison with the PLA fibers. These modifications of the properties were more noticeable in the case of the acrylated PMS, which also provided readily available functional groups at the surface for further chemical reactions, such as the Michael addition or crosslinking processes. Full article

(This article belongs to the Special Issue Polyester-Based Materials)

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19 pages, 50285 KiB

Open AccessArticle

Combining Materials Obtained by 3D-Printing and Electrospinning from Commercial Polylactide Filament to Produce Biocompatible Composites

by Pablo Romero-Araya, Victor Pino, Ariel Nenen, Verena Cárdenas, Francisca Pavicic, Pamela Ehrenfeld, Guillaume Serandour, Judit G. Lisoni, Ignacio Moreno-Villoslada and Mario E. Flores

Polymers 2021, 13(21), 3806; https://0-doi-org.brum.beds.ac.uk/10.3390/polym13213806 - 03 Nov 2021

Cited by 11 | Viewed by 3712

Abstract

The design of scaffolds to reach similar three-dimensional structures mimicking the natural and fibrous environment of some cells is a challenge for tissue engineering, and 3D-printing and electrospinning highlights from other techniques in the production of scaffolds. The former is a well-known additive manufacturing technique devoted to the production of custom-made structures with mechanical properties similar to tissues and bones found in the human body, but lacks the resolution to produce small and interconnected structures. The latter is a well-studied technique to produce materials possessing a fibrillar structure, having the advantage of producing materials with tuned composition compared with a 3D-print. Taking the advantage that commercial 3D-printers work with polylactide (PLA) based filaments, a biocompatible and biodegradable polymer, in this work we produce PLA-based composites by blending materials obtained by 3D-printing and electrospinning. Porous PLA fibers have been obtained by the electrospinning of recovered PLA from 3D-printer filaments, tuning the mechanical properties by blending PLA with small amounts of polyethylene glycol and hydroxyapatite. A composite has been obtained by blending two layers of 3D-printed pieces with a central mat of PLA fibers. The composite presented a reduced storage modulus as compared with a single 3D-print piece and possessing similar mechanical properties to bone tissues. Furthermore, the biocompatibility of the composites is assessed by a simulated body fluid assay and by culturing composites with 3T3 fibroblasts. We observed that all these composites induce the growing and attaching of fibroblast over the surface of a 3D-printed layer and in the fibrous layer, showing the potential of commercial 3D-printers and filaments to produce scaffolds to be used in bone tissue engineering. Full article

(This article belongs to the Special Issue Polyester-Based Materials)

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13 pages, 1151 KiB

Open AccessArticle

Increased Comfort of Polyester Fabrics

by Meritxell Martí, Jaime Gisbert-Paya, Mª Ángeles Bonet-Aracil, Petar Jovančić, Manuel J. Lis and Luisa Coderch

Polymers 2021, 13(17), 3010; https://0-doi-org.brum.beds.ac.uk/10.3390/polym13173010 - 06 Sep 2021

Cited by 3 | Viewed by 3594

Abstract

The hydrophilicity of fibers is directly related to the comfort of a fabric and represents one of the most important aspects of a textile. Therefore, polyester (PES) modification has focused on an increase in moisture content and a subsequent improvement of the user’s experience. Based on the glycerol hygroscopic properties, the main objective has been the enhancement of the hydrophilicity of polyester by glycerol treatments. Furthermore, microwave irradiation and alkaline treatment have been applied, in order to increase glycerol adhesion. Treated PES samples were characterized by performing moisture content, negative ion, water diffusion and water vapor resistance analyses. The effect of different treatment conditions such as bath ratio (1/10 or 1/15), temperature (40, 60 or 100 °C), time (2 or 5 min) and microwave radiation intensity (300 or 500 W) was evaluated. The moisture content of treated PES results indicated that by decreasing the bath ratio and increasing the time and temperature the moisture gain can reach almost 14%, which can be easily related to increases in the weight of the fiber. The treatment with alkali was done and led to the highest moisture increase. Treatment with 500 W microwave irradiation led to higher glycerol retention after rinsing. Different experimental conditions were applied to the glycerol-treated PES fabrics, and a clear improvement in moisture content was obtained increasing the comfort. The results were compared with the ones obtained for cotton and wool, where the moisture is higher than non treated PES. Full article

(This article belongs to the Special Issue Polyester-Based Materials)

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27 pages, 3107 KiB

Open AccessArticle

3,4-Ethylenedioxythiophene (EDOT) End-Group Functionalized Poly-ε-caprolactone (PCL): Self-Assembly in Organic Solvents and Its Coincidentally Observed Peculiar Behavior in Thin Film and Protonated Media

by Anca-Dana Bendrea, Luminita Cianga, Gabriela-Liliana Ailiesei, Elena-Laura Ursu, Demet Göen Colak and Ioan Cianga

Polymers 2021, 13(16), 2720; https://0-doi-org.brum.beds.ac.uk/10.3390/polym13162720 - 14 Aug 2021

Cited by 6 | Viewed by 3058

Abstract

End-group functionalization of homopolymers is a valuable way to produce high-fidelity nanostructured and functional soft materials when the structures obtained have the capacity for self-assembly (SA) encoded in their structural details. Herein, an end-functionalized PCL with a π-conjugated EDOT moiety, (EDOT-PCL), designed exclusively from hydrophobic domains, as a functional “hydrophobic amphiphile”, was synthesized in the bulk ROP of ε-caprolactone. The experimental results obtained by spectroscopic methods, including NMR, UV-vis, and fluorescence, using DLS and by AFM, confirm that in solvents with extremely different polarities (chloroform and acetonitrile), EDOT-PCL presents an interaction- and structure-based bias, which is strong and selective enough to exert control over supramolecular packing, both in dispersions and in the film state. This leads to the diversity of SA structures, including spheroidal, straight, and helical rods, as well as orthorhombic single crystals, with solvent-dependent shapes and sizes, confirming that EDOT-PCL behaves as a “block-molecule”. According to the results from AFM imaging, an unexpected transformation of micelle-type nanostructures into single 2D lamellar crystals, through breakout crystallization, took place by simple acetonitrile evaporation during the formation of the film on the mica support at room temperature. Moreover, EDOT-PCL’s propensity for spontaneous oxidant-free oligomerization in acidic media was proposed as a presumptive answer for the unexpected appearance of blue color during its dissolution in CDCl₃ at a high concentration. FT-IR, UV-vis, and fluorescence techniques were used to support this claim. Besides being intriguing and unforeseen, the experimental findings concerning EDOT-PCL have raised new and interesting questions that deserve to be addressed in future research. Full article

(This article belongs to the Special Issue Polyester-Based Materials)

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16 pages, 2078 KiB

Open AccessArticle

Improved Mechanical, Thermal, and Hydrophobic Properties of PLA Modified with Alkoxysilanes by Reactive Extrusion Process

by Elena Torres, Aide Gaona, Nadia García-Bosch, Miguel Muñoz, Vicent Fombuena, Rosana Moriana and Ana Vallés-Lluch

Polymers 2021, 13(15), 2475; https://0-doi-org.brum.beds.ac.uk/10.3390/polym13152475 - 27 Jul 2021

Cited by 6 | Viewed by 2551

Abstract

An eco-friendly strategy for the modification of polylactic acid (PLA) surface properties, using a solvent-free process, is reported. Reactive extrusion (REX) allowed the formation of new covalent bonds between functional molecules and the PLA polymeric matrix, enhancing its mechanical properties and modifying surface hydrophobicity. To this end, the PLA backbone was modified using two alkoxysilanes, phenyltriethoxysilane and N-octyltriethoxysilane. The reactive extrusion process was carried out under mild conditions, using melting temperatures between 150 and 180 °C, 300 rpm as screw speed, and a feeding rate of 3 kg·h⁻¹. To complete the study, flat tapes of neat and functionalized PLA were obtained through monofilament melt extrusion to quantify the enhancement of mechanical properties and hydrophobicity. The results verified that PLA modified with 3 wt% of N-octyltriethoxysilane improves mechanical and thermal properties, reaching Young’s modulus values of 4.8 GPa, and PLA hydrophobic behavior, with values of water contact angle shifting from 68.6° to 82.2°. Full article

(This article belongs to the Special Issue Polyester-Based Materials)

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19 pages, 10769 KiB

Open AccessEditor’s ChoiceArticle

Electrospun Nanosystems Based on PHBV and ZnO for Ecological Food Packaging

by Maria Râpă, Maria Stefan, Paula Adriana Popa, Dana Toloman, Cristian Leostean, Gheorghe Borodi, Dan Cristian Vodnar, Magdalena Wrona, Jesús Salafranca, Cristina Nerín, Daniel Gabriel Barta, Maria Suciu, Cristian Predescu and Ecaterina Matei

Polymers 2021, 13(13), 2123; https://0-doi-org.brum.beds.ac.uk/10.3390/polym13132123 - 28 Jun 2021

Cited by 18 | Viewed by 2916

Abstract

The electrospun nanosystems containing poly(3-hydroxybutyrate-co-3-hydroxyvalerate) (PHBV) and 1 wt% Fe doped ZnO nanoparticles (NPs) (with the content of dopant in the range of 0–1 wt% Fe) deposited onto polylactic acid (PLA) film were prepared for food packaging application. They were investigated by scanning electron microscopy (SEM), energy dispersive X-ray (EDX), Fourier transform infrared spectroscopy (FT-IR), X-ray diffraction (XRD), antimicrobial analysis, and X-ray photoelectron spectrometry (XPS) techniques. Migration studies conducted in acetic acid 3% (wt/wt) and ethanol 10% (v/v) food simulants as well as by the use of treated ashes with 3% HNO₃ solution reveal that the migration of Zn and Fe falls into the specific limits imposed by the legislation in force. Results indicated that the PLA/PHBV/ZnO:Fex electrospun nanosystems exhibit excellent antibacterial activity against the Pseudomonas aeruginosa (ATCC-27853) due to the generation of a larger amount of perhydroxyl (˙OOH) radicals as assessed using electron paramagnetic resonance (EPR) spectroscopy coupled with a spin trapping method. Full article

(This article belongs to the Special Issue Polyester-Based Materials)

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20 pages, 2953 KiB

Open AccessArticle

Biobased Thermoplastic Elastomers: Structure-Property Relationship of Poly(hexamethylene 2,5-furanodicarboxylate)-Block-Poly(tetrahydrofuran) Copolymers Prepared by Melt Polycondensation

by Sandra Paszkiewicz, Izabela Irska, Agata Zubkiewicz, Anna Szymczyk, Elżbieta Piesowicz, Zbigniew Rozwadowski and Krzysztof Goracy

Polymers 2021, 13(3), 397; https://0-doi-org.brum.beds.ac.uk/10.3390/polym13030397 - 27 Jan 2021

Cited by 19 | Viewed by 3467

Abstract

A series of poly(hexamethylene 2,5-furanodicarboxylate)-block-poly(tetrahydrofuran) (PHF-b-F-pTHF) copolymers were synthesized using a two-stage procedure, employing transesterification and polycondensation. The content of pTHF flexible segments varied from 25 to 75 wt.%. ¹H nuclear magnetic resonance (NMR) and Fourier transformed infrared spectroscopy (FTIR) analyses were applied to confirm the molecular structure of the materials. Differential scanning calorimetry (DSC), dynamic mechanical measurements (DMTA), and X-ray diffraction (XRD) allowed characterizing the supramolecular structure of the synthesized copolymers. SEM analysis was applied to show the differences in the block copolymers’ morphologies concerning their chemical structure. The influence of the number of flexible segments in the copolymers on the phase transition temperatures, thermal properties, as well as the thermo-oxidative and thermal stability was analyzed. TGA analysis, along with tensile tests (static and cyclic), confirmed the utilitarian performance of the synthesized bio-based materials. It was found that an increase in the amount of pTHF caused the increase of both number-average and weight-average molecular weights and intrinsic viscosities, and at the same time causing the shift of the values of phase transition temperatures toward lower ones. Besides, PHF-b-F-pTHF containing 75 wt.% of F-pTHF units was proved to be a promising thermoplastic shape memory polymer (SMP) with a switching temperature of 20 °C. Full article

(This article belongs to the Special Issue Polyester-Based Materials)

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Review

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49 pages, 3809 KiB

Open AccessReview

Special Features of Polyester-Based Materials for Medical Applications

by Raluca Nicoleta Darie-Niță, Maria Râpă and Stanisław Frąckowiak

Polymers 2022, 14(5), 951; https://0-doi-org.brum.beds.ac.uk/10.3390/polym14050951 - 27 Feb 2022

Cited by 30 | Viewed by 6296

Abstract

This article presents current possibilities of using polyester-based materials in hard and soft tissue engineering, wound dressings, surgical implants, vascular reconstructive surgery, ophthalmology, and other medical applications. The review summarizes the recent literature on the key features of processing methods and potential suitable combinations of polyester-based materials with improved physicochemical and biological properties that meet the specific requirements for selected medical fields. The polyester materials used in multiresistant infection prevention, including during the COVID-19 pandemic, as well as aspects covering environmental concerns, current risks and limitations, and potential future directions are also addressed. Depending on the different features of polyester types, as well as their specific medical applications, it can be generally estimated that 25–50% polyesters are used in the medical field, while an increase of at least 20% has been achieved since the COVID-19 pandemic started. The remaining percentage is provided by other types of natural or synthetic polymers; i.e., 25% polyolefins in personal protection equipment (PPE). Full article

(This article belongs to the Special Issue Polyester-Based Materials)

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