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Recent Developments in Biodegradable and Biobased Polymers

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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 (20 January 2023) | Viewed by 29846

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Special Issue Editor

Prof. Dr. Shinichi Sakurai

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Department of Biobased Materials Science, Kyoto Institute of Technology, Kyoto 606-8585, Japan
Interests: nanostructure analysis; small-angle X-ray scattering; block copolymer; polymer physics; polymer crystallization; pattern formation
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Special Issue Information

Dear Colleagues,

Biodegradable polymers are considered promising materials to solve the problem of microplastic pollution in marine environments. In addition, biobased polymers utilizing plants can be used to reduce the concentration of carbon dioxide in the atmosphere and can contribute to carbon neutralization. However, these polymers have some crucial drawbacks such as poor crystallizability and insufficient mechanical properties, compared to commodity polymers synthesized using monomers from fossil fuels. Therefore, many research studies have been devoted to improving their crystallizability and mechanical properties. For crystallizability, the addition of a nucleation agent, diluent, or plasticizer has been reported. To ameliorate the mechanical properties, block copolymerization and polymer blending are main strategies, but it is important to use additives derived from natural sources and components of block copolymers or polymer blends that are biobased and/or biodegradable. In this context, new biobased monomers and synthetic routes of biobased polymers from such biobased monomers should be investigated. The biodegradable behaviors of such new biobased polymers should also be examined. This Special Issue focuses on these topics, including biomedical applications and recent developments in biodegradable and biobased polymers.

Prof. Dr. Shinichi Sakurai
Guest Editor

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Keywords

biobased monomer
synthesis
biodegradable behavior
mechanical property
crystallization
biobased additives
block copolymerization
polymer blending
biomedical application

Related Special Issue

Recent Developments in Biodegradable and Biobased Polymers II in Polymers (1 article)

Published Papers (13 papers)

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Research

12 pages, 302 KiB

Open AccessArticle

Effects of Dietary Rare Earth Chitosan Chelate on Performance, Egg Quality, Immune and Antioxidant Capacity, and Intestinal Digestive Enzyme Activity of Laying Hens

by Xinxin Lu, Xinyu Chang, Haijun Zhang, Jing Wang, Kai Qiu and Shugeng Wu

Polymers 2023, 15(7), 1600; https://doi.org/10.3390/polym15071600 - 23 Mar 2023

Cited by 3 | Viewed by 1136

Abstract

Rare earth chitosan chelate salt (RECC) is a potential feed additive and is a product of the chelation effect between rare earth ions and chitosan. This research study aims to explore the effects of dietary RECC on performance, egg quality, intestinal digestive function, and the immune and antioxidant capacity of laying hens in the late phase of production. A total of 360 56-week-old Dawu Jinfeng laying hens were randomly allotted into four treatment groups with six replicates per treatment and 15 birds per replicate. The laying hens were fed the basal diet supplemented with, respectively, 0 (control: CON), 100 (R1), 200 (R2), and 400 (R3) mg/kg for 8 weeks. Dietary RECC significantly improved average daily feed intake (ADFI) and average daily egg yield in both linear and quadratic manner (p < 0.05). In addition, albumen height and HU were improved significantly (p < 0.05) in a dose-dependent manner of RECC. In addition, a significant decrease (p < 0.05) in serum TP, IgA, and MDA for the R1 group and IgG in the R2 group were notable, while the increase in serum TP and decrease in T-AOC were found for R3 dietary group compared to CON (p < 0.05). The level of intestinal IL-2 and TNF-α was decreased by dietary RECC (p < 0.01). The activities of the digestive enzyme (α-Amylase, lipase, and Trypsin) showed a quadratic change with an increase and then decrease in response to increasing dose of RECC, 200 mg/kg RECC significantly increased the activity of lipase and Trypsin (p < 0.01). Supplementation of dietary RECC at low doses compared to higher doses impacted positive effects on the antioxidant capacity and immune function (p < 0.05). The utilization of RECC as a feed additive in the diet of aged laying hens exerted beneficial effects on egg production, albumen quality, humoral immunity, inflammatory response, and activity of digestive enzymes. Thus, the regulation of antioxidant capacity and duodenal function via increased enzyme activity and immune and inflammatory response were critical to the improvement of laying performance and egg quality in aged hens. The optimal supplemental dose is 100–200 mg/kg. Full article

(This article belongs to the Special Issue Recent Developments in Biodegradable and Biobased Polymers)

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12 pages, 1459 KiB

Open AccessArticle

Mechanical Properties of Protein-Based Hydrogels Derived from Binary Protein Mixtures—A Feasibility Study

by Sandra Haas and Jürgen Hubbuch

Polymers 2023, 15(4), 964; https://doi.org/10.3390/polym15040964 - 15 Feb 2023

Viewed by 1352

Abstract

Hydrogels based on natural polymers such as proteins are considered biocompatible and, therefore, represent an interesting class of materials for application in the field of biomedicine and high-performance materials. However, there is a lack of understanding of the proteins which are able to form hydrogel networks by photoinduced dityrosine crosslinking as well as a profound knowledge of the formed network itself and the mechanisms which are responsible for the resulting mechanical properties of such protein-based hydrogels. In this study, casein, bovine serum albumin, α-amylase, and a hydrophobic elastin-like protein were used to prepare binary protein mixtures with defined concentration ratios. After polymerization, the mechanical properties of the resulting homopolymeric and copolymeric hydrogels were determined using rheological methods depending on the protein shares used. In additional uniaxial compression tests, the fracture strain was shown to be independent of the protein shares, while hydrogel toughness and compressive strength were increased for protein-based hydrogels containing casein. Full article

(This article belongs to the Special Issue Recent Developments in Biodegradable and Biobased Polymers)

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16 pages, 3661 KiB

Open AccessArticle

Effect of Styrene-Maleic Anhydride Copolymer on Properties of PBST/PLA Blends

by Qing Zhang, Yongguang Gao, Baojing Luo, Yan Cui, Shili Shu, Wei Chen and Lei Wang

Polymers 2023, 15(4), 952; https://doi.org/10.3390/polym15040952 - 15 Feb 2023

Cited by 6 | Viewed by 2017

Abstract

Poly(butylene succinate-butylene terephthalate) (PBST) and polylactic acid (PLA) are both biodegradable polymeric materials. PBST has good ductility but low strength, while PLA exhibits high strength but poor toughness. Based on the complementary mechanical properties of the two polymers, PBST/PLA blends were prepared by melt blending in the mixing chamber of a torque rheometer using styrene-maleic anhydride copolymer (PSMA) as a compatibilizer. The effects of different contents of PSMA on the crystalline properties, thermal properties, mechanical properties, rheological behavior, and morphology of PBST/PLA blends were investigated. The results showed that the addition of PSMA improved the compatibility between PBST and PLA. When the amount of PSMA is 3–4 wt%, the comprehensive mechanical properties of the blends are optimal, and the tensile strength was increased by 61.7% compared with the binary blend without PSMA. Additionally, rheological tests illustrated that the blends exhibited a typical shear-thinning behavior and belonged to pseudoplastic non-Newtonian fluids. Full article

(This article belongs to the Special Issue Recent Developments in Biodegradable and Biobased Polymers)

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12 pages, 2404 KiB

Open AccessArticle

Screening of Polyethylene-Degrading Bacteria from Rhyzopertha Dominica and Evaluation of Its Key Enzymes Degrading Polyethylene

by Yao Zhang, Yuan Lin, Hongmei Gou, Xu Feng, Xian Zhang and Lijuan Yang

Polymers 2022, 14(23), 5127; https://doi.org/10.3390/polym14235127 - 25 Nov 2022

Cited by 10 | Viewed by 2046

Abstract

Polyethylene (PE) is widely used, and it has caused serious environmental problems due to its difficult degradation. At present, the mechanism of PE degradation by microorganisms is not clear, and the related enzymes of PE degradation need to be further explored. In this study, Acinetobacter baumannii Rd-H2 was obtained from Rhizopertha dominica, which had certain degradation effect on PE plastic. The degradation performance of the strains was evaluated by weight loss rate, SEM, ATR/FTIR, WCA, and GPC. The multi-copper oxidase gene abMco, which may be one of the key genes for PE degradation, was analyzed and successfully expressed in E. coli. The laccase activity of the gene was determined, and the enzyme activity was up to 159.82 U/L. The optimum temperature and pH of the enzyme are 45 °C and 4.5 respectively. It shows good stability at 30–45 °C. Cu²⁺ can activate the enzyme. The abMCO was used to degrade polyethylene film, showing a good degradation effect, proving that the enzyme could be the key to degrading PE. Full article

(This article belongs to the Special Issue Recent Developments in Biodegradable and Biobased Polymers)

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16 pages, 2756 KiB

Open AccessArticle

Coordinative Chain Transfer Polymerization of Sustainable Terpene Monomers Using a Neodymium-Based Catalyst System

by Teresa Córdova, Francisco Javier Enríquez-Medrano, Eduardo Martínez Cartagena, Arnulfo Banda Villanueva, Luis Valencia, Edgar Nazareo Cabrera Álvarez, Ricardo López González and Ramón Díaz-de-León

Polymers 2022, 14(14), 2907; https://doi.org/10.3390/polym14142907 - 17 Jul 2022

Cited by 4 | Viewed by 1852

Abstract

The present investigation involves the coordinative chain transfer polymerization (CCTP) of biobased terpenes in order to obtain sustainable polymers from myrcene (My) and farnesene (Fa), using the ternary Ziegler–Natta catalyst system comprising [NdV₃]/[Al(i-Bu)₂H]/[Me₂SiCl₂] and Al(i-Bu)₂H, which acts as cocatalyst and chain transfer agent (CTA). The polymers were produced with a yield above 85% according to the monomeric consumption at the end of the reaction, and the kinetic examination revealed that the catalyst system proceeded with a reversible chain transfer mechanism in the presence of 15–30 equiv. of CTA. The resulting polyterpenes showed narrow molecular weight distributions (M_w/M_n = 1.4–2.5) and a high percent of 1,4-cis microstructure in the presence of 1 equiv. of Me₂SiCl₂, having control of the molecular weight distribution in Ziegler–Natta catalytic systems that maintain a high generation of 1,4-cis microstructure. Full article

(This article belongs to the Special Issue Recent Developments in Biodegradable and Biobased Polymers)

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15 pages, 4860 KiB

Open AccessArticle

A Green Approach for the Synthesis of Silver Nanoparticle-Embedded Chitosan Bionanocomposite as a Potential Device for the Sustained Release of the Itraconazole Drug and Its Antibacterial Characteristics

by Saruchi, Manpreet Kaur, Vaneet Kumar, Ayman A. Ghfar and Sadanand Pandey

Polymers 2022, 14(9), 1911; https://doi.org/10.3390/polym14091911 - 07 May 2022

Cited by 13 | Viewed by 1794

Abstract

The present research work intended to demonstrate the green synthesis of silver nanoparticles (AgNPs) using the plant extract Saccharum officinarum, and then the development of chitosan–silver (CH-Ag) bionanocomposite. The synthesized AgNPs were characterized using UV spectroscopy, Fourier transform infrared (FTIR), and transmission electron microscopy (TEM). The maximum absorption spectrum peak was observed at 420 nm, revealing the formation of AgNPs by the stem extract of S. officinarum. The AgNPs sizes were in the range of 10–50 nm. Itraconazole is an antifungal that is used as a novel drug to study its release through synthesized bionanocomposite. Different kinetic models, such as zero order, first order, Korsmeyer–Peppas, Hixson–Crowell and Higuchi, were used to study the drug release profile from the synthesized CH-Ag bionanocomposite. The first-order kinetic model showed the best fit for the drug release with the maximum regression coefficient value. The antibacterial activity of the synthesized CH-Ag bionanocomposite was examined against Bacillus cereus, Staphylococcus, and Escherichia coli, and it was shown to be efficient against these strains. Full article

(This article belongs to the Special Issue Recent Developments in Biodegradable and Biobased Polymers)

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14 pages, 3686 KiB

Open AccessArticle

Utility of Thermal Cross-Linking in Stabilizing Hydrogels with Beta-Tricalcium Phosphate and/or Epigallocatechin Gallate for Use in Bone Regeneration Therapy

by Beiyuan Gao, Yoshitomo Honda, Yoichi Yamada, Tomonari Tanaka, Yoshihiro Takeda, Takayuki Nambu and Shunsuke Baba

Polymers 2022, 14(1), 40; https://doi.org/10.3390/polym14010040 - 23 Dec 2021

Cited by 3 | Viewed by 2427

Abstract

β-tricalcium phosphate (β-TCP) granules are commonly used materials in dentistry or orthopedic surgery. However, further improvements are required to raise the operability and bone-forming ability of β-TCP granules in a clinical setting. Recently, we developed epigallocatechin gallate (EGCG)-modified gelatin sponges as a novel biomaterial for bone regeneration. However, there is no study on using the above material for preparing hydrogel incorporating β-TCP granules. Here, we demonstrate that vacuum heating treatment induced thermal cross-linking in gelatin sponges modified with EGCG and incorporating β-TCP granules (vhEc-GS-β) so that the hydrogels prepared from vhEc-GS-β showed high stability, β-TCP granule retention, operability, and cytocompatibility. Additionally, microcomputed tomography morphometry revealed that the hydrogels from vhEc-GS-β had significantly higher bone-forming ability than β-TCP alone. Tartrate-resistant acid phosphatase staining demonstrated that the number of osteoclasts increased at three weeks in defects treated with the hydrogels from vhEc-GS-β compared with that around β-TCP alone. The overall results indicate that thermal cross-linking treatment for the preparation of sponges (precursor of hydrogels) can be a promising process to enhance the bone-forming ability. This insight should provide a basis for the development of novel materials with good operativity and bone-forming ability for bone regenerative medicine. Full article

(This article belongs to the Special Issue Recent Developments in Biodegradable and Biobased Polymers)

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16 pages, 3657 KiB

Open AccessArticle

Preparation and Characterization of Calcium Cross-Linked Starch Monolithic Cryogels and Their Application as Cost-Effective Green Filters

by Chanita Boonkanon, Kharittha Phatthanawiwat, Laemthong Chuenchom, Nareumon Lamthornkit, Tarawee Taweekarn, Worawit Wongniramaikul and Aree Choodum

Polymers 2021, 13(22), 3975; https://doi.org/10.3390/polym13223975 - 17 Nov 2021

Cited by 9 | Viewed by 2720

Abstract

Monolithic cryogels from starch were successfully synthesized and applied as alternative biodegradable filters for the first time. Rice flour was cross-linked with Ca²⁺ from limewater during gelatinization before being frozen and then thawed for three cycles. The resultant material was then soaked in ethanol for 3 h before incubation at 80 °C for 1 h, yielding monolithic material with interconnected pores in sizes of 51 ± 18 to 52 ± 15 µm without any need of freeze-drying. The cryogels possessed macroporous structure with specific surface areas from 1.1 to 4.3 m²g⁻¹, they could adsorb water from 599 ± 27 to 635 ± 59% of their dry weight with low swelling ratios of 6.0 ± 0.3 to 6.4 ± 0.6 g_water/g_cryogel, and could be applied as biofilters to remove suspended particles and reduce the light absorption of water sample from 25 ± 3 to 96 ± 5%. The prepared biofilters can be re-used up to three times, although they cost only USD 0.0004/piece. Complete weight loss resulted from burial in soil for 30 days, indicating environmentally friendly biodegradation and potential for environmental applications. Full article

(This article belongs to the Special Issue Recent Developments in Biodegradable and Biobased Polymers)

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21 pages, 11119 KiB

Open AccessArticle

Controllable Release of Povidone-Iodine from Networked Pectin@Carboxymethyl Pullulan Hydrogel

by Hossam E. Emam and Amina L. Mohamed

Polymers 2021, 13(18), 3118; https://doi.org/10.3390/polym13183118 - 15 Sep 2021

Cited by 24 | Viewed by 2984

Abstract

Povidone-iodine (PI) is a common antiseptic reagent which is used for skin infections and wound healing. The control release of PI is quite important to heal the deep and intense wounds. Herein, the preparation of biodegradable pectin@carboxymethyl pullulan (Pe@CMP) hydrogel was carried out and applied for controllable release of PI. CMP was synthesized by interaction of monochloroacetic acid with pullulan at different ratios. The Pe@CMP hydrogel was then prepared by crosslinking of pectin with CMP in presence of glutaraldehyde as cross linker. After carboxymethylation, COOH contents were enlarged to be 24.2–51.2 mmol/kg and degree of substitution was 0.44–0.93. The rheological properties of Pe@CMP hydrogel were enlarged by increment of pectin ratio. Swelling ratio in water (16.0–18.0%) was higher than that of artificial sweat (11.7–13.2%). Pe@CMP hydrogel containing 20% pectin, exhibited the lowest release and 57.7% from PI was released within 360 min. The biological activity of the released PI was monitored to be highly efficient. The kinetic of release was fitted well to the first ordered reaction and Higuchi models. The mechanism of release was explained by the swelling of hydrogel. The networked structure of hydrogel was opened by swelling and PI was released from the outer pores followed by inner pores, achieving the controllable release. Full article

(This article belongs to the Special Issue Recent Developments in Biodegradable and Biobased Polymers)

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11 pages, 25420 KiB

Open AccessArticle

Properties Enhancement of High Molecular Weight Polylactide Using Stereocomplex Polylactide as a Nucleating Agent

by Purba Purnama, Muhammad Samsuri and Ihsan Iswaldi

Polymers 2021, 13(11), 1725; https://doi.org/10.3390/polym13111725 - 25 May 2021

Cited by 14 | Viewed by 2332

Abstract

As one of the most attractive biopolymers nowadays in terms of their sustainability, degradability, and material tune-ability, the improvement of polylactide (PLA) homopolymer properties by studying the utilization of stereocomplex polylactide (s-PLA) effectively and efficiently is needed. In this sense, we have studied the utilization of s-PLA compared to poly D-lactide (PDLA) homopolymers as a nucleating agent for PLA homopolymers. The mechanical and thermal properties and crystallization behavior of PLA homopolymers in the presence of nucleating agents have been evaluated using a universal testing machine, differential scanning calorimeter, and X-ray diffractometer instruments, respectively. PDLA and s-PLA materials can be used to increase the thermal and mechanical properties of poly L-lactide (PLLA) homopolymers. The s-PLA materials increased the mechanical properties by increasing crystallinity of the PLLA homopolymers. PLLA/s-PLA enhanced mechanical properties to a certain level (5% s-PLA content), then decreased them due to higher s-PLA materials affecting the brittleness of the blends. PDLA homopolymers increased mechanical properties by forming stereocomplex PLA with PLLA homopolymers. Non-isothermal and isothermal evaluation showed that s-PLA materials were more effective at enhancing PLLA homopolymer properties through nucleating agent mechanism. Full article

(This article belongs to the Special Issue Recent Developments in Biodegradable and Biobased Polymers)

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17 pages, 3908 KiB

Open AccessArticle

Development of Polylactic Acid Thermoplastic Starch Formulations Using Maleinized Hemp Oil as Biobased Plasticizer

by Alejandro Lerma-Canto, Jaume Gomez-Caturla, María Herrero-Herrero, Daniel Garcia-Garcia and Vicent Fombuena

Polymers 2021, 13(9), 1392; https://doi.org/10.3390/polym13091392 - 25 Apr 2021

Cited by 26 | Viewed by 3621

Abstract

In this study, hemp seed oil was reacted with maleic anhydride in an ene reaction to obtain maleinized hemp seed oil (MHO). The use of MHO as a plasticizer and compatibilizer has been studied for polylactic acid (PLA) and thermoplastic starch (TPS) blends (80/20, respectively). By mechanical, thermal and morphological characterizations, the addition of MHO provides a dual effect, acting as plasticizer and compatibilizer between these two partially miscible biopolymers. The addition of MHO up to 7.5 phr (parts by weight of MHO per hundred parts of PLA and TPS) revealed a noticeable increase in the ductile properties, reaching an elongation at break 155% higher than the PLA/TPS blend. Furthermore, contrary to what has been observed with maleinized oils such as linseed oil, the thermal properties do not decrease significantly as a result of the plasticizing effect, due to the compatibilizing behavior of the MHO and the natural antioxidants present in the oil. Finally, a disintegration test was carried out in aerobic conditions at 58 °C, for 24 days, to demonstrate that the incorporation of the MHO, although causing a slight delay, does not impair the biodegradability of the blend, obtaining total degradation in 24 days. Full article

(This article belongs to the Special Issue Recent Developments in Biodegradable and Biobased Polymers)

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20 pages, 7952 KiB

Open AccessArticle

Degradability of Polyurethanes and Their Blends with Polylactide, Chitosan and Starch

by Joanna Brzeska, Agnieszka Tercjak, Wanda Sikorska, Barbara Mendrek, Marek Kowalczuk and Maria Rutkowska

Polymers 2021, 13(8), 1202; https://doi.org/10.3390/polym13081202 - 08 Apr 2021

Cited by 9 | Viewed by 2023

Abstract

One of the methods of making traditional polymers more environmentally friendly is to modify them with natural materials or their biodegradable, synthetic equivalents. It was assumed that blends with polylactide (PLA), polysaccharides: chitosan (Ch) and starch (St) of branched polyurethane (PUR) based on synthetic poly([R,S]-3-hydroxybutyrate) (R,S-PHB) would degrade faster in the processes of hydrolysis and oxidation than pure PUR. For the sake of simplicity in the publication, all three modifiers: commercial PLA, Ch created by chemical modification of chitin and St are called bioadditives. The samples were incubated in a hydrolytic and oxidizing environment for 36 weeks and 11 weeks, respectively. The degradation process was assessed by observation of the chemical structure as well as the change in the mass of the samples, their molecular weight, surface morphology and thermal properties. It was found that the PUR samples with the highest amount of R,S-PHB and the lowest amount of polycaprolactone triol (PCL_triol) were degraded the most. Moreover, blending with St had the greatest impact on the susceptibility to degradation of PUR. However, the rate of weight loss of the samples was low, and after 36 weeks of incubation in the hydrolytic solution, it did not exceed 7% by weight. The weight loss of Ch and PLA blends was even smaller. However, a significant reduction in molecular weight, changes in morphology and changes in thermal properties indicated that the degradation of the samples should occur quickly after this time. Therefore, when using these polyurethanes and their blends, it should be taken into account that they should decompose slowly in their initial life. In summary, this process can be modified by changing the amount of R,S-PHB, the degree of cross-linking, and the type and amount of second blend component added (bioadditives). Full article

(This article belongs to the Special Issue Recent Developments in Biodegradable and Biobased Polymers)

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16 pages, 4411 KiB

Open AccessArticle

Fabrication and Properties of Electrospun Collagen Tubular Scaffold Crosslinked by Physical and Chemical Treatments

by Xuefei Chen, Jie Meng, Huaizhong Xu, Masaya Shinoda, Masanori Kishimoto, Shinichi Sakurai and Hideki Yamane

Polymers 2021, 13(5), 755; https://doi.org/10.3390/polym13050755 - 28 Feb 2021

Cited by 13 | Viewed by 2293

Abstract

Tissue engineered scaffold was regarded as a promising approach instead of the autograft. In this study, small diameter electrospun collagen tubular scaffold with random continuous smooth nanofibers was successfully fabricated. However, the dissolution of collagen in concentrated aqueous (conc. aq.) acetic acid caused to the serious denaturation of collagen. A novel method ammonia treatment here was adopted which recovered the collagen triple helix structure according to the analysis of IR spectra. Further dehydrothermal (DHT) and glutaraldehyde (GTA) treatments were applied to introduce the crosslinks to improve the properties of collagen tube. The nanofibrous structure of collagen tube in a wet state was preserved by the crosslinking treatments. Swelling ratio and weight loss decreased by at least two times compared to those of the untreated collagen tube. Moreover, tensile strength was significantly enhanced by DHT treatment (about 0.0076 cN/dTex) and by GTA treatment (about 0.075 cN/dTex). In addition, the surface of crosslinked collagen tube kept the hydrophilic property. These results suggest that DHT and GTA treatments can be utilized to improve the properties of electrospun collagen tube which could become a suitable candidate for tissue engineered scaffold. Full article

(This article belongs to the Special Issue Recent Developments in Biodegradable and Biobased Polymers)

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