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A special issue of International Journal of Molecular Sciences (ISSN 1422-0067). This special issue belongs to the section "Materials Science".

Deadline for manuscript submissions: closed (28 February 2019) | Viewed by 25318

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Special Issue Editor

Dr. Eric Pollet

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Guest Editor

ICPEES-ECPM, Université de Strasbourg (UniStra), 25 Rue Becquerel, F-67087 Strasbourg CEDEX 2, France
Interests: biobased monomers and polymers; biodegradable polymers; polymer nanocomposites and biocomposites; enzymatic polymerization; polysaccharides; polyesters

Special Issue Information

Dear Colleagues,

Over the past few decades, the worldwide production of synthetic polymers (human-made polymers commonly produced from fossil-based chemicals) has increased almost exponentially and, thus, has led to significant issues. On the one hand, the high volatility of oil prices and limited reserves of fossil resources are now important drawbacks. On the other hand, polymer synthesis from fossil resources may contribute to greenhouse gas emissions and the main use of these polymers for short term applications results in persistent plastics debris accumulating in the environment. It is, thus, necessary to develop more eco-friendly polymers to reduce the current dependence on fossil resources and also decrease the production of pollutants. The development of biodegradable and/or biobased polymers has thus gained increasing interest over the past twenty years to meet such growing demand for sustainable development. Biodegradable polymers can be obtained from either renewable or fossil sources while bio-based polymers are either biodegradable or durable (non-biodegradable). Biodegradable polymers such as polysaccharides or aliphatic polyesters are particularly significant as a potential solution for the reduction of plastic wastes pollution. On the other hand, bio-based polymers, synthesized from renewable resources using chemical methods or even enzymatic routes as a greener approach, have recently received considerable attention in an effort to replace petroleum-based plastics with polymers displaying much lower ecological footprint.

This Special Issue of International Journal of Material Science will thus aim at presenting the most recent findings in the field of biodegradable and/or bio-based polymeric materials.

Dr. Eric Pollet
Guest Editor

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Keywords

Biobased polymers
Biodegradable polymers
Bioplastics
Biopolymers
Monomers from biomass
Renewable resources
Sustainable materials
Polysaccharides
Biodegradable polyesters

Published Papers (6 papers)

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Research

15 pages, 1869 KiB

Open AccessArticle

Block Copolyesters Containing 2,5-Furan and trans-1,4-Cyclohexane Subunits with Outstanding Gas Barrier Properties

by Giulia Guidotti, Laura Genovese, Michelina Soccio, Matteo Gigli, Andrea Munari, Valentina Siracusa and Nadia Lotti

Int. J. Mol. Sci. 2019, 20(9), 2187; https://doi.org/10.3390/ijms20092187 - 02 May 2019

Cited by 27 | Viewed by 3244

Abstract

Biopolymers are gaining increasing importance as substitutes for plastics derived from fossil fuels, especially for packaging applications. In particular, furanoate-based polyesters appear as the most credible alternative due to their intriguing physic/mechanical and gas barrier properties. In this study, block copolyesters containing 2,5-furan and trans-1,4-cyclohexane moieties were synthesized by reactive blending, starting from the two parent homopolymers: poly(propylene furanoate) (PPF) and poly(propylene cyclohexanedicarboxylate) (PPCE). The whole range of molecular architectures, from long block to random copolymer with a fixed molar composition (1:1 of the two repeating units) was considered. Molecular, thermal, tensile, and gas barrier properties of the prepared materials were investigated and correlated to the copolymer structure. A strict dependence of the functional properties on the copolymers’ block length was found. In particular, short block copolymers, thanks to the introduction of more flexible cyclohexane-containing co-units, displayed high elongation at break and low elastic modulus, thus overcoming PPF’s intrinsic rigidity. Furthermore, the exceptionally low gas permeabilities of PPF were further improved due to the concomitant action of the two rings, both capable of acting as mesogenic groups in the presence of flexible aliphatic units, and thus responsible for the formation of 1D/2D ordered domains, which in turn impart outstanding barrier properties. Full article

(This article belongs to the Special Issue Biobased and/or Biodegradable Polymeric Materials)

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17 pages, 3387 KiB

Open AccessArticle

Chitosan Hydrogel Beads Supported with Ceria for Boron Removal

by Joanna Kluczka, Gabriela Dudek, Alicja Kazek-Kęsik and Małgorzata Gnus

Int. J. Mol. Sci. 2019, 20(7), 1567; https://doi.org/10.3390/ijms20071567 - 28 Mar 2019

Cited by 17 | Viewed by 2997

Abstract

In this study, a chitosan hydrogel supported with ceria (labelled Ce-CTS) was prepared by an encapsulation technique and used for the efficient removal of excess B(III) from aqueous solutions. The functionalisation of chitosan with Ce(IV) and the improvement in the adsorptive behaviour of the hydrogel were determined by SEM-EDS, FTIR, XRD, and inductively coupled plasma optical emission spectrometer (ICP-OES) analyses and discussed. The results demonstrate that Ce-CTS removes boric acid from aqueous solutions more efficiently than either cerium dioxide hydrate or raw chitosan beads, the precursors of the Ce-CTS biosorbent. The maximum adsorption capacity of 13.5 ± 0.9 mg/g was achieved at pH 7 after 24 h. The equilibrium data of boron adsorption on Ce-CTS fitted the Freundlich isotherm model, while the kinetic data followed the Elovich pseudo-second-order model, which indicated that the process was non-homogeneous. The dominant mechanism of removal was the reaction between boric acid molecules and hydroxyl groups bound to the ceria chelated by chitosan active centres. Due to its high efficiency in removing boron, good regeneration capacity and convenient form, Ce-CTS may be considered a promising biosorbent in water purification. Full article

(This article belongs to the Special Issue Biobased and/or Biodegradable Polymeric Materials)

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17 pages, 2542 KiB

Open AccessArticle

Cellulose-starch Hybrid Films Plasticized by Aqueous ZnCl₂ Solution

by Xiaoqin Shang, Huihua Jiang, Qingling Wang, Peng Liu and Fengwei Xie

Int. J. Mol. Sci. 2019, 20(3), 474; https://doi.org/10.3390/ijms20030474 - 22 Jan 2019

Cited by 14 | Viewed by 4506

Abstract

Starch and cellulose are two typical natural polymers from plants that have similar chemical structures. The blending of these two biopolymers for materials development is an interesting topic, although how their molecular interactions could influence the conformation and properties of the resultant materials has not been studied extensively. Herein, the rheological properties of cellulose/starch/ZnCl₂ solutions were studied, and the structures and properties of cellulose-starch hybrid films were characterized. The rheological study shows that compared with starch (containing mostly amylose), cellulose contributed more to the solution’s viscosity and has a stronger shear-thinning behavior. A comparison between the experimental and calculated zero-shear-rate viscosities indicates that compact complexes (interfacial interactions) formed between cellulose and starch with ≤50 wt % cellulose content, whereas a loose structure (phase separation) existed with ≥70 wt % cellulose content. For starch-rich hybrid films prepared by compression molding, less than 7 wt % of cellulose was found to improve the mechanical properties despite the reduced crystallinity of the starch; for cellulose-rich hybrid films, a higher content of starch reduced the material properties, although the chemical interactions were not apparently influenced. It is concluded that the mechanical properties of biopolymer films were mainly affected by the structural conformation, as indicated by the rheological results. Full article

(This article belongs to the Special Issue Biobased and/or Biodegradable Polymeric Materials)

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18 pages, 3840 KiB

Open AccessArticle

Original Macromolecular Architectures Based on poly(ε-caprolactone) and poly(ε-thiocaprolactone) Grafted onto Chitosan Backbone

by Cüneyt H. Ünlü, Eric Pollet and Luc Avérous

Int. J. Mol. Sci. 2018, 19(12), 3799; https://doi.org/10.3390/ijms19123799 - 29 Nov 2018

Cited by 8 | Viewed by 3234

Abstract

Polyester and/or polythioester grafted chitosan copolymers were synthesized. For that, poly(ε-caprolactone) (PCL), poly(ε-thiocaprolactone) (PTCL), and their copolymers were first synthesized by ring opening polymerization. Copolymers with caprolactone:thiocaprolactone (CL:TCL) molar ratios of 2:1, 1:1, 1:2 were synthesized. All of the synthesized macromolecular architectures were characterized using different spectral (Fourier transform infrared (FTIR), proton nuclear magnetic resonance (¹H-NMR), X-Ray diffraction (XRD)) and thermal (Differential scanning calorimetry (DSC), Thermogravimetric analysis (TGA)) methods. Grafting was then performed according two distinct routes: (i) using a blend of both homopolymers (PCL and PTCL) or (ii) using pre-synthesized copolymers with controlled CL:TCL ratios. Hexamethylene diisocyanate was used as a grafting/coupling agent through urethane bonds with high yield. Grafting preferentially occurred at sulfur sites. The results indicated that PTCL is more reactive and favorable than PCL for grafting onto chitosan. With the homopolymers blend grafting route, the corresponding materials mostly had a higher PTCL portion than expected. To obtain polyester grafted chitosan with a determined CL:TCL ratio, the copolymer grafting route would yield better results. Full article

(This article belongs to the Special Issue Biobased and/or Biodegradable Polymeric Materials)

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14 pages, 3724 KiB

Open AccessArticle

Biological and Mechanical Properties of Platelet-Rich Fibrin Membranes after Thermal Manipulation and Preparation in a Single-Syringe Closed System

by Dorottya Kardos, István Hornyák, Melinda Simon, Adél Hinsenkamp, Bence Marschall, Róbert Várdai, Alfréd Kállay-Menyhárd, Balázs Pinke, László Mészáros, Olga Kuten, Stefan Nehrer and Zsombor Lacza

Int. J. Mol. Sci. 2018, 19(11), 3433; https://doi.org/10.3390/ijms19113433 - 01 Nov 2018

Cited by 42 | Viewed by 5446

Abstract

Platelet-rich fibrin (PRF) membrane is a three-dimensional biodegradable biopolymer, which consists of platelet derived growth factors enhancing cell adhesion and proliferation. It is widely used in soft and hard tissue regeneration, however, there are unresolved problems with its clinical application. Its preparation needs open handling of the membranes, it degrades easily, and it has a low tensile strength which does not hold a suture blocking wider clinical applications of PRF. Our aim was to produce a sterile, suturable, reproducible PRF membrane suitable for surgical intervention. We compared the biological and mechanical properties of PRF membranes created by the classical glass-tube and those that were created in a single-syringe closed system (hypACT Inject), which allowed aseptic preparation. HypACT Inject device produces a PRF membrane with better handling characteristics without compromising biological properties. Freeze-thawing resulted in significantly higher tensile strength and higher cell adhesion at a lower degradation rate of the membranes. Mesenchymal stem cells seeded onto PRF membranes readily proliferated on the surface of fresh, but even better on freeze/thawed or freeze-dried membranes. These data show that PRF membranes can be made sterile, more uniform and significantly stronger which makes it possible to use them as suturable surgical membranes. Full article

(This article belongs to the Special Issue Biobased and/or Biodegradable Polymeric Materials)

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13 pages, 1943 KiB

Open AccessArticle

Chemo-Enzymatic Synthesis of Renewable Sterically-Hindered Phenolic Antioxidants with Tunable Polarity from Lignocellulose and Vegetal Oil Components

by Louis Hollande, Sandra Domenek and Florent Allais

Int. J. Mol. Sci. 2018, 19(11), 3358; https://doi.org/10.3390/ijms19113358 - 26 Oct 2018

Cited by 13 | Viewed by 5247

Abstract

Despite their great antioxidant activities, the use of natural phenols as antioxidant additives for polyolefins is limited owing to their weak thermal stability and hydrophilic character. Herein, we report a sustainable chemo-enzymatic synthesis of renewable lipophilic antioxidants specifically designed to overcome these restrictions using naturally occurring ferulic acid (found in lignocellulose) and vegetal oils (i.e., lauric, palmitic, stearic acids, and glycerol) as starting materials. A predictive Hansen and Hildebrand parameters-based approach was used to tailor the polarity of newly designed structures. A specific affinity of Candida antarctica lipase B (CAL-B) towards glycerol was demonstrated and exploited to efficiently synthesized the target compounds in yields ranging from 81 to 87%. Antiradical activity as well as radical scavenging behavior (H atom-donation, kinetics) of these new fully biobased additives were found superior to that of well-established, commercially available fossil-based antioxidants such as Irganox 1010^® and Irganox 1076^®. Finally, their greater thermal stabilities (302 < T_d5% < 311 °C), established using thermal gravimetric analysis, combined with their high solubilities and antioxidant activities, make these novel sustainable phenolics a very attractive alternative to current fossil-based antioxidant additives in polyolefins. Full article

(This article belongs to the Special Issue Biobased and/or Biodegradable Polymeric Materials)

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