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Biodegradable Polymers - Where We Are and Where to Going

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

Deadline for manuscript submissions: closed (31 October 2019) | Viewed by 44392

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Special Issue Editors

Prof. Dr. Marek M. Kowalczuk

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Guest Editor

Centre of Polymer and Carbon Materials Polish Academy of Sciences, PL-41819 Zabrze, Poland
Interests: biocompatible and biodegradable polymer systems; polymer mass spectrometry; bioactive oligomers; controlled drug delivery systems; ring-opening polymerization; forensic engineering of advanced polymeric materials
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Prof. Dr. Grażyna Adamus

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Centre of Polymer and Carbon Materials, Polish Academy of Sciences, M. Curie-Skłodowskiej 34, 41-819 Zabrze, Poland
Interests: polymers from renewable resources; synthesis of functional polymers; structure–property relationships; novel polymeric materials of controlled biodegradability; application of mass spectrometry techniques to the structural study of synthetic polymers at the molecular level
Special Issues, Collections and Topics in MDPI journals

Special Issue Information

Dear Colleagues,

We are just at the beginning of cleaning up the effects of the development of classic plastics. The development of biodegradable polymers possesses boundless significance and opens up new possibilities for a future sustainable society. The use of biodegradable polymers is of great importance for many applications. Biodegradable polymers include natural polymers from plants, such as starch, polymers produced by microorganisms (polyhydroxyalkanoate, PHA), polymers whose monomers have a natural origin (polylactide, PLA), and synthetic polymers, such as aliphatic–aromatic co-polyesters. PHA is a group of biopolyesters that has a wide range of applications. Extensive progress has been made in our understanding of PHA biosynthesis, and currently it is possible to engineer bacterial strains to produce PHA with desired properties. Moreover, the chemical modification of PHA, which introduces functional groups that cannot be easily achieved by bioconversion processes, are a valuable challenge, since chemically-modified PHA can be utilized as a multifunctional biomaterial. However, further studies are still needed in order to define and minimize the potential failure of novel biodegradable polymer products for specific applications.

This Special Issue comprises already published papers devoted to biodegradable polymers for environmental and medical applications and welcomes reviews, full papers and short communications highlighting various aspects of the current trends in this area.

Prof. Marek M. Kowalczuk
Prof. Grażyna Adamus
Guest Editors

Keywords

novel synthetic approaches for biodegradable polymers
structure–property relationships of biodegradable polymers
characterization of biodegradable polymers at the molecular level
biodegradable polymeric packages of food and cosmetics
biodegradable polymeric mulch films

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Published Papers (7 papers)

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Research

12 pages, 2636 KiB

Open AccessArticle

Anionic Polymerization of β-Butyrolactone Initiated with Sodium Phenoxides. The Effect of the Initiator Basicity/Nucleophilicity on the ROP Mechanism

by Adrian Domiński, Tomasz Konieczny, Magdalena Zięba, Magdalena Klim and Piotr Kurcok

Polymers 2019, 11(7), 1221; https://doi.org/10.3390/polym11071221 - 22 Jul 2019

Cited by 21 | Viewed by 5409

Abstract

It was shown that selected sodium phenoxide derivatives with different basicity and nucleophilicity, such as sodium p-nitrophenoxide, p-chlorophenoxide, 1-napthoxide, phenoxide and p-methoxyphenoxide, are effective initiators in anionic ring-opening polymerization (AROP) of β-butyrolactone in mild conditions. It was found that phenoxides as initiators in anionic ring-opening polymerization of β-butyrolactone behave as strong nucleophiles, or weak nucleophiles, as well as Brønsted bases. The resulting polyesters possessing hydroxy, phenoxy and crotonate initial groups are formed respectively by the attack of phenoxide anion at (i) C2 followed by an elimination reaction with hydroxide formation, (ii) C4 and (iii) abstraction of acidic proton at C3. The obtained poly(3-hydroxybutyrate) possesses carboxylate growing species. The ratio of the observed initial groups strongly depends on the basicity and nucleophilicity of the sodium phenoxide derivative used as initiator. The proposed mechanism of this polymerization describes the reactions leading to formation of observed end groups. Moreover, the possibility of formation of a crotonate group during the propagation step of this polymerization is also discussed. Full article

(This article belongs to the Special Issue Biodegradable Polymers - Where We Are and Where to Going)

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16 pages, 3684 KiB

Open AccessEditor’s ChoiceArticle

Degradation Behavior In Vitro of Carbon Nanotubes (CNTs)/Poly(lactic acid) (PLA) Composite Suture

by Shuqiang Liu, Gaihong Wu, Xiaogang Chen, Xiaofang Zhang, Juanjuan Yu, Mingfang Liu, Yao Zhang and Peng Wang

Polymers 2019, 11(6), 1015; https://doi.org/10.3390/polym11061015 - 8 Jun 2019

Cited by 62 | Viewed by 7318

Abstract

Poly(lactic acid) (PLA) suture can be absorbed by the human body, and so have wide applications in modern surgery operations. The degradation period of PLA suture is expected to meet with the healing time of different types of wounds. In order to control the degradation period of the PLA suture, the carbon nanotubes (CNTs) were composited with PLA suture, and the degradation experiment in vitro was performed on sutures. The structure and properties of sutures during degradation, such as surface morphology, breaking strength, elongation, mass and chemical structure, were tracked and analyzed. The results indicated that the degradation brought about surface defects and resulted in 13.5 weeks for the strength valid time of the original PLA suture. By contrast, the strength valid time of the CNTs/PLA suture was increased to 26.6 weeks. Whilst the toughness of both the pure PLA and CNTs/PLA sutures decreased rapidly and almost disappeared after 3 to 4 weeks of degradation. The mass loss demonstrated that the time required for complete degradation of the two sutures was obviously different, the pure PLA suture 49 weeks, while CNTs/PLA sutures 63 to 73 weeks. The research proved that CNTs delayed PLA degradation and prolonged its strength valid time in degradation. Full article

(This article belongs to the Special Issue Biodegradable Polymers - Where We Are and Where to Going)

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15 pages, 4079 KiB

Open AccessArticle

(Bio)degradable Polymeric Materials for Sustainable Future—Part 2: Degradation Studies of P(3HB-co-4HB)/Cork Composites in Different Environments

by Sebastian Jurczyk, Marta Musioł, Michał Sobota, Magdalena Klim, Anna Hercog, Piotr Kurcok, Henryk Janeczek and Joanna Rydz

Polymers 2019, 11(3), 547; https://doi.org/10.3390/polym11030547 - 22 Mar 2019

Cited by 18 | Viewed by 4714

Abstract

The degree of degradation of pure poly(3-hydroxybutyrate-co-4-hydroxybutyrate) [P(3HB-co-4HB)] and its composites with cork incubated under industrial and laboratory composting conditions was investigated. The materials were parallelly incubated in distilled water at 70 °C as a reference experiment (abiotic condition). It was demonstrated that addition of the cork into polyester strongly affects the matrix crystallinity. It influences the composite degradation independently on the degradation environment. Moreover, the addition of the cork increases the thermal stability of the obtained composites; this was related to a smaller reduction in molar mass during processing. This phenomenon also had an influence on the composite degradation process. The obtained results suggest that the addition of cork as a natural filler in various mass ratios to the composites enables products with different life expectancies to be obtained. Full article

(This article belongs to the Special Issue Biodegradable Polymers - Where We Are and Where to Going)

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15 pages, 3598 KiB

Open AccessArticle

Thermal and Mechanical Properties of Biocomposites Made of Poly(3-hydroxybutyrate-co-3-hydroxyvalerate) and Potato Pulp Powder

by Maria Cristina Righetti, Patrizia Cinelli, Norma Mallegni, Andreas Stäbler and Andrea Lazzeri

Polymers 2019, 11(2), 308; https://doi.org/10.3390/polym11020308 - 12 Feb 2019

Cited by 28 | Viewed by 4274

Abstract

The thermal and mechanical properties of biocomposites of poly(3-hydroxybutyrate-co-3-hydroxyvalerate) (PHBV) containing 5 wt % of valerate units, with 20 wt % of potato pulp powder were investigated in order (i) to obtain information on possible miscibility/compatibility between the biopolymers and the potato pulp, and (ii) to quantify how the addition of this filler modifies the properties of the polymeric material. The potato pulp powder utilized is a residue of processing for the production and extraction of starch. The final aim of this study is the preparation of PHBV based materials with reduced cost, thanks to biomass valorization, in agreement with the circular economy policy, as result of the incorporation of agricultural organic waste. The results showed that the potato pulp powder does not act as reinforcement, but rather as filler for the PHBV polymeric matrix. A moderate loss in mechanical properties is detected (decrease in elastic modulus, tensile strength and elongation at break), which regardless still meets the technical requirements indicated for rigid packaging production. In order to improve the mechanical response of the PHBV/potato pulp powder biocomposites, surface treatment of the potato pulp powder with bio-based and petroleum-based waxes was investigated. Good enhancement of the mechanical properties was achieved with the natural carnauba and bee waxes. Full article

(This article belongs to the Special Issue Biodegradable Polymers - Where We Are and Where to Going)

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7 pages, 1343 KiB

Open AccessCommunication

Effect of Lecithin on the Spontaneous Crystallization of Enzymatically Synthesized Short-Chain Amylose Molecules into Spherical Microparticles

by Carlos Andres Morales Letona, Ke Luo, Ki-Baek Jeong, Hazzel Joy Adra, Cheon-Seok Park and Young-Rok Kim

Polymers 2019, 11(2), 264; https://doi.org/10.3390/polym11020264 - 4 Feb 2019

Cited by 19 | Viewed by 4284

Abstract

Here, we report a facile and effective one-pot approach to prepare uniform amylose-based polymeric microparticles (PMPs) through enzymatic synthesis of short-chain amylose (SCA) followed by spontaneous self-assembly of the SCA in the presence of lecithin. The effect of lecithin on nucleation and growth kinetics of amylose microparticles was investigated by monitoring the turbidity of reaction solution and the size of particles over the course of the self-assembly process. The results suggest that lecithin played a critical role in controlling the self-assembly kinetics to form uniform amylose microparticles through steric stabilization of the growing particles and diffusion-limited growth effect. The crystallinity of amylose microparticles was not affected by lecithin, implying that lecithin did not disrupt the crystal structure within the particle and would mainly be present on the surface of the microparticles. Considering its biodegradable and biocompatible nature, the amylose-based microparticles would find a range of useful applications in the area of food, cosmetics, medicine, chromatography and other related materials sciences. Full article

(This article belongs to the Special Issue Biodegradable Polymers - Where We Are and Where to Going)

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16 pages, 4183 KiB

Open AccessArticle

Effect of Chemical Composition Variant and Oxygen Plasma Treatments on the Wettability of PLGA Thin Films, Synthesized by Direct Copolycondensation

by Muhammad Ayyoob and Young Jun Kim

Polymers 2018, 10(10), 1132; https://doi.org/10.3390/polym10101132 - 12 Oct 2018

Cited by 41 | Viewed by 6676

Abstract

The synthesis of high molecular weight poly (lactic-co-glycolic) acid (PLGA) copolymers via direct condensation copolymerization is itself a challenging task. Moreover, some of the characteristic properties of polylactide (PLA)-based biomaterials, such as brittleness, hydrophobicity, and longer degradation time, are not suitable for certain biomedical applications. However, such properties can be altered by the copolymerization of PLA with other biodegradable monomers, such as glycolic acid. A series of high molecular weight PLGAs were synthesized through the direct condensation copolymerization of lactic and glycolic acids, starting from 0 to 50 mol% of glycolic acid, and the wettability of its films was monitored as a function of the feed molar ratio. Copolymerization was performed in the presence of a bi-catalytic system using stannous chloride dihydrate and methanesulfonic acid (MSA). The viscosity average molecular weight of the resulting PLGA was in the range of 80k to 135k g/mol. The PLGA films were prepared using the solvent casting technique, and were treated with oxygen plasma for 2 min. The water contact angle of the PLGA films was determined before and after the oxygen plasma treatments, and it was observed that the wettability increased with an increase in the glycolic acid contents, however, the manifolds increased after 2 min of oxygen plasma treatments. Full article

(This article belongs to the Special Issue Biodegradable Polymers - Where We Are and Where to Going)

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22 pages, 3565 KiB

Open AccessArticle

The Microbial Production of Polyhydroxyalkanoates from Waste Polystyrene Fragments Attained Using Oxidative Degradation

by Brian Johnston, Iza Radecka, David Hill, Emo Chiellini, Vassilka Ivanova Ilieva, Wanda Sikorska, Marta Musioł, Magdalena Zięba, Adam A. Marek, Daniel Keddie, Barbara Mendrek, Surila Darbar, Grazyna Adamus and Marek Kowalczuk

Polymers 2018, 10(9), 957; https://doi.org/10.3390/polym10090957 - 29 Aug 2018

Cited by 71 | Viewed by 10409

Abstract

Excessive levels of plastic waste in our oceans and landfills indicate that there is an abundance of potential carbon sources with huge economic value being neglected. These waste plastics, through biological fermentation, could offer alternatives to traditional petrol-based plastics. Polyhydroxyalkanoates (PHAs) are a group of plastics produced by some strains of bacteria that could be part of a new generation of polyester materials that are biodegradable, biocompatible, and, most importantly, non-toxic if discarded. This study introduces the use of prodegraded high impact and general polystyrene (PS0). Polystyrene is commonly used in disposable cutlery, CD cases, trays, and packaging. Despite these applications, some forms of polystyrene PS remain financially and environmentally expensive to send to landfills. The prodegraded PS0 waste plastics used were broken down at varied high temperatures while exposed to ozone. These variables produced PS flakes (PS1–3) and a powder (PS4) with individual acid numbers. Consequently, after fermentation, different PHAs and amounts of biomass were produced. The bacterial strain, Cupriavidus necator H16, was selected for this study due to its well-documented genetic profile, stability, robustness, and ability to produce PHAs at relatively low temperatures. The accumulation of PHAs varied from 39% for prodegraded PS0 in nitrogen rich media to 48% (w/w) of dry biomass with the treated PS. The polymers extracted from biomass were analyzed using nuclear magnetic resonance (NMR) and electrospray ionization tandem mass spectrometry (ESI-MS/MS) to assess their molecular structure and properties. In conclusion, the PS0–3 specimens were shown to be the most promising carbon sources for PHA biosynthesis; with 3-hydroxybutyrate and up to 12 mol % of 3-hydroxyvalerate and 3-hydroxyhexanoate co-monomeric units generated. Full article

(This article belongs to the Special Issue Biodegradable Polymers - Where We Are and Where to Going)

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