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A special issue of Materials (ISSN 1996-1944). This special issue belongs to the section "Biomaterials".

Deadline for manuscript submissions: closed (31 May 2021) | Viewed by 63090

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Dr. Tomonari Tanaka

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Department of Biobased Materials Science, Graduate School of Science and Technology, Kyoto Institute of Technology, Matsugasaki, Sakyo-ku, Kyoto 606-8585, Japan
Interests: glycomaterials; glycotechnology; chemical and enzymatic synthesis; green chemistry; biobased materials

Special Issue Information

Dear Colleagues,

Biobased polymers, which are defined as sustainable polymeric materials produced from renewable biomass resources, are becoming some of the most important core materials in science and technology. Within this century, they are expected to replace the conventional oil-based polymers synthesized from fossil resources. To create a sustainable society, new technology and further development are required.

In this Special Issue, we aim to present valuable findings regarding “biobased polymers”. This research area covers diverse fields, including organic chemistry, polymer chemistry, microbiology, biotechnology, chemical engineering, materials science, and materials physics, and others.

Considering your prominent contribution to this extensively studied research topic, I would like to cordially invite you to submit an article to this Special Issue. Original articles, communications, and review articles discussing the latest findings in the field of biobased polymers are all welcome. I would be very grateful if you could consider being one of our authors.

Dr. Tomonari Tanaka
Guest Editor

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Keywords

sustainable materials
non-fossil resources
biomass
eco-friendly
natural polymers

Published Papers (10 papers)

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Research

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18 pages, 5234 KiB

Open AccessArticle

Chitosan as a Protective Matrix for the Squaraine Dye

by Halina Kaczmarek, Patryk Rybczyński, Piotr Maćczak, Aleksander Smolarkiewicz-Wyczachowski and Marta Ziegler-Borowska

Materials 2021, 14(5), 1171; https://doi.org/10.3390/ma14051171 - 2 Mar 2021

Cited by 5 | Viewed by 1705

Abstract

Chitosan was used as a protective matrix for the photosensitive dye-squaraine (2,4-bis[4-(dimethylamino)phenyl]cyclobutane-1,3-diol). The physicochemical properties of the obtained systems, both in solution and in a solid-state, were investigated. However, it was found that diluted chitosan solutions with a few percent additions of dye show an intense fluorescence, which is suppressed in the solid-state. This is related to the morphology of the heterogeneous modified chitosan films. The important advantage of using a biopolymer matrix is the prevention of dye degradation under the influence of high energy ultraviolet (UV) radiation while the dye presence improves the chitosan heat resistance. It is caused by mutual interactions between macromolecules and dye. Owing to the protective action of chitosan, the dye release in liquid medium is limited. Chitosan solutions with a few percent additions of squaraine can be used in biomedical imaging thanks to the ability to emit light, while chitosan films can be protective coatings resistant to high temperatures and UV radiation. Full article

(This article belongs to the Special Issue Biobased Polymers)

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20 pages, 3028 KiB

Open AccessArticle

Chemical Changes of Wood Treated with Caffeine

by Patrycja Kwaśniewska-Sip, Magdalena Woźniak, Wojciech Jankowski, Izabela Ratajczak and Grzegorz Cofta

Materials 2021, 14(3), 497; https://doi.org/10.3390/ma14030497 - 21 Jan 2021

Cited by 17 | Viewed by 3361

Abstract

Earlier studies have revealed that wood treated with caffeine was effectively protected against decay fungi and molds. However, there is a need to establish how the caffeine molecule behaves after wood impregnation and how it can protect wood. The objective of the research was to characterize the interaction between caffeine and Scots pine (Pinus sylvestris L.) wood as well as to assess the stability of the alkaloid molecule in lignocellulosic material. For this purpose, an elementary analyzer was used to assess the nitrogen concentration in the treated wood. The results showed that caffeine is easily removed from the wood structure through large amounts of water. The changes occurring in the wood structure after impregnation were evaluated with regard to the results obtained by Fourier transform infrared (FTIR) spectroscopy of two model mixtures with caffeine and cellulose or lignin for the purpose of conducting a comparison with the spectrum of impregnated and non-impregnated samples. The observed changes in FTIR spectra involve the intensity of the C=O(6) caffeine carbonyl group and signals from guaiacyl units. It might indicate favorable interactions between caffeine and lignin. Additionally, molecular simulation of the caffeine’s interaction with the guaiacyl β-O-4 lignin model compound characteristic for the lignin structure using computational studies was performed. Consequently, all analyses confirmed that caffeine may interact with the methylene group derived from the aromatic rings of the guaiacyl group of lignin. In summary, scanning electron microscope (SEM) observations suggest that caffeine was accumulated in the lignin-rich areas of the primary walls. Full article

(This article belongs to the Special Issue Biobased Polymers)

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8 pages, 2751 KiB

Open AccessArticle

Biobased Poly(itaconic Acid-co-10-Hydroxyhexylitaconic Acid)s: Synthesis and Thermal Characterization

by Yuji Aso, Mei Sano, Ryoki Yada, Tomonari Tanaka, Takashi Aoki, Hitomi Ohara, Takahiro Kusukawa, Keiji Matsumoto and Kazuhito Wada

Materials 2020, 13(12), 2707; https://doi.org/10.3390/ma13122707 - 14 Jun 2020

Cited by 9 | Viewed by 3261

Abstract

Renewable vinyl compounds itaconic acid (IA) and its derivative 10-hydroxyhexylitaconic acid (10-HHIA) are naturally produced by fungi from biomass. This provides the opportunity to develop new biobased polyvinyls from IA and 10-HHIA monomers. In this study, we copolymerized these monomers at different ratios through free radical aqueous polymerization with potassium peroxodisulfate as an initiator, resulting in poly(IA-co-10-HHIA)s with different monomer compositions. We characterized the thermal properties of the polymers by thermogravimetric analysis (TGA) and Fourier-transform infrared spectroscopy (FT-IR). The nuclear magnetic resonance analysis and the gel permeation chromatography showed that the polymerization conversion, yield, and the molecular weights (weight-averaged Mw and number-averaged Mn) of the synthesized poly(IA-co-10-HHIA)s decreased with increasing 10-HHIA content. It is suggested that the hydroxyhexyl group of 10-HHIA inhibited the polymerization. The TGA results indicated that the poly(IA-co-10-HHIA)s continuously decomposed as temperature increased. The FT-IR analysis suggested that the formation of the hydrogen bonds between the carboxyl groups of IA and 10-HHIA in the polymer chains was promoted by heating and consequently the polymer dehydration occurred. To the best of our knowledge, this is the first time that biobased polyvinyls were synthesized using naturally occurring IA derivatives. Full article

(This article belongs to the Special Issue Biobased Polymers)

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18 pages, 2724 KiB

Open AccessArticle

Thermal and Morphological Properties of Poly(L-Lactic Acid)/Poly(D-Lactic Acid)-B-Polycaprolactone Diblock Copolymer Blends

by Eckhard Weidner, Stephan Kabasci, Rodion Kopitzky and Philip Mörbitz

Materials 2020, 13(11), 2550; https://doi.org/10.3390/ma13112550 - 3 Jun 2020

Cited by 4 | Viewed by 2523

Abstract

Due to the brittle nature of poly(lactic acid) many attempts have been made to flexibilize this polyester for applications such as thin films and foils. However, due to complex phase behavior, many drawbacks for plasticizer and blend components are described. To overcome miscibility, post crystallization and migration issues a principle of click-chemistry was employed to change the molecular characteristics from external to internal plasticization by fixation of a plastisizing unit with help of a stereocomplex crystallization. Hydroxyl terminated polycaprolactone oligomers were used as a macroinitiator for the ring opening polymerization of d-lactide, resulting in blockcopolymers with plasticizing unit polycaprolactone and compatibilizing poly(d-lactic acid)-blocks. The generated block copolymers were blended with a poly(l-lactic acid)-matrix and formed so called stereocomplex crystals. In comparison to unbound polycaprolactone the polycaprolactone blocks show a lower migration tendency regarding a solution test in toluene. Besides that, trapping the plasticizing units via stereocomplex also improves the efficiency of the plasticizer. In comparison to polymer blends with the same amount of non-bonded polycaprolactone oligomers of the same molecular weight, block copolymers with poly(d-lactic acid) and polycaprolactone can shift the glass transition temperature to lower values. This effect can be explained by the modulated crystallization of the polycaprolactone-blocks trapped into the matrix, so that a higher effective amount can interact with the poly(l-lactic acid)-matrix. Full article

(This article belongs to the Special Issue Biobased Polymers)

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15 pages, 5062 KiB

Open AccessArticle

Effect of the Application of a Dehydrothermal Treatment on the Structure and the Mechanical Properties of Collagen Film

by Xuefei Chen, Lingling Zhou, Huaizhong Xu, Masaki Yamamoto, Masaya Shinoda, Masanori Kishimoto, Tomonari Tanaka and Hideki Yamane

Materials 2020, 13(2), 377; https://doi.org/10.3390/ma13020377 - 14 Jan 2020

Cited by 34 | Viewed by 4796

Abstract

Dehydrothermal (DHT) treatment was used to improve the properties of collagen casings because of its non-cytotoxicity. Understanding the effects of DHT treatment on the structure and mechanical properties of collagen films is beneficial to developing satisfying collagen casings. Herein, DHT treatment with various temperatures (85–145 °C) and timescales (1–7 days) were investigated. It was clarified that the chemical crosslinking covalent bond between collagen molecules was formed after the DHT treatment. Crosslinking density increased with increasing DHT treatment temperatures, contributing to the increase of tensile strength up to over three times of that of the untreated collagen film. The increased crosslinking density was also found when increasing the DHT treatment time, and the maximum was obtained in 3 days. Further DHT treatment time did not change the crosslinking density. The damage in the triple helix structure and the self-assembly of collagen molecules were observed from IR and SAXS. The extent of denaturation increased with increasing DHT treatment temperature and time, although the effect of the DHT treatment time on the denaturation was more moderate. When the DHT treatment temperature was as high as 145 °C or the DHT treatment time exceeded 5 days, serious denaturation occurs, leading to the deterioration of mechanical properties. Full article

(This article belongs to the Special Issue Biobased Polymers)

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18 pages, 5861 KiB

Open AccessArticle

Releasing Behavior of Lipopolysaccharide from Gelatin Modulates Inflammation, Cellular Senescence, and Bone Formation in Critical-Sized Bone Defects in Rat Calvaria

by Jianxin Zhao, Yoshitomo Honda, Tomonari Tanaka, Yoshiya Hashimoto and Naoyuki Matsumoto

Materials 2020, 13(1), 95; https://doi.org/10.3390/ma13010095 - 23 Dec 2019

Cited by 13 | Viewed by 3479

Abstract

Lipopolysaccharide (LPS) is a well-known strong inducer of inflammation. However, there is little information regarding how LPS-release behavior affects cellular senescence at the affected area. In this paper, we demonstrate that a vacuum-heating technique (dehydrothermal treatment) can be utilized to prepare an LPS sustained-release gelatin sponge (LS-G). LPS sustained release from gelatin leads to the long-term existence of senescent cells in critical-sized bone defects in rat calvaria. Three types of gelatin sponges were prepared in this study: a medical-grade gelatin sponge with extremely low LPS levels (MG), LS-G, and a LPS rapid-release gelatin sponge (LR-G). Histological (H-E) and immunohistochemical (COX-2, p16, and p21) staining were utilized to evaluate inflammatory reactions and cellular senescence one to three weeks after surgery. Soft X-ray imaging was utilized to estimate new bone formation in the defects. The LR-G led to stronger swelling and COX-2 expression in defects compared to the MG and LS-G at 1 week. Despite a small inflammatory reaction, LS-G implantation led to the long-term existence of senescent cells and hampered bone formation compared to the MG and LR-G. These results suggest that vacuum heating is a viable technique for preparing different types of materials for releasing bacterial components, which is helpful for developing disease models for elucidating cellular senescence and bone regeneration. Full article

(This article belongs to the Special Issue Biobased Polymers)

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8 pages, 2386 KiB

Open AccessArticle

Preparation of Reswellable Amorphous Porous Celluloses through Hydrogelation from Ionic Liquid Solutions

by Satoshi Idenoue, Yoshitaka Oga, Daichi Hashimoto, Kazuya Yamamoto and Jun-ichi Kadokawa

Materials 2019, 12(19), 3249; https://doi.org/10.3390/ma12193249 - 4 Oct 2019

Cited by 10 | Viewed by 2547

Abstract

In this study, we have performed the preparation of reswellable amorphous porous celluloses through regeneration from hydrogels. The cellulose hydrogels were first prepared from solutions with an ionic liquid, 1-butyl-3-methylimidazolium chloride (BMIMCl), in different concentrations. Lyophilization of the hydrogels efficiently produced the regenerated celluloses. The powder X-ray diffraction and scanning electron microscopic measurements of the products suggest an amorphous structure and porous morphology, respectively. Furthermore, the pore sizes of the regenerated celluloses, or in turn, the network sizes of cellulose chains in the hydrogels, were dependent on the concentrations of the initially prepared solutions with BMIMCl, which also affected the tensile mechanical properties. It was suggested that the dissolution states of the cellulose chains in the solutions were different, in accordance with the concentrations, which representatively dominated the pore and network sizes of the above materials. When the porous celluloses were immersed in water, reswelling was observed to regenerate the hydrogels. Full article

(This article belongs to the Special Issue Biobased Polymers)

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14 pages, 4900 KiB

Open AccessArticle

Structural Evolution in Isothermal Crystallization Process of Poly(L-lactic acid) Enhanced by Silk Fibroin Nano-Disc

by Amit Kumar Pandey, Vimal Katiyar, Hideaki Takagi, Nobutaka Shimizu, Noriyuki Igarashi, Sono Sasaki and Shinichi Sakurai

Materials 2019, 12(11), 1872; https://doi.org/10.3390/ma12111872 - 10 Jun 2019

Cited by 10 | Viewed by 3466

Abstract

The nucleating effect of silk fibroin nano-disc (SFN) on the crystallization behavior of poly(L-lactic acid) (PLLA) was investigated by simultaneous synchrotron small- and wide-angle X-ray scattering measurements. For the isothermal crystallization at 110 °C from the melt, the induction period of the PLLA specimens containing 1% SFN was reduced compared to that of the neat specimens, indicating the acceleration of the nucleation of PLLA. The final degree of crystallinity was also increased, and the crystallization half-time was decreased, which indicates that the overall crystallization process was accelerated. Furthermore, the final value of the crystallite size (the lateral size of the crystalline lamella) was slightly lower for the specimens containing 1% SFN than that for the PLLA neat specimen, although the crystallites started growing much earlier. However, it was found that there was no effect of SFN on the growth rate of the crystallite size. The lamellar thickening process was also accelerated with a clear overshooting phenomenon with the inclusion of 1% SFN. As for the polymorphism, the α’ phase is dominant with about 96%, but a small amount of the α phase (4%) is found to exist. It was found that the SFN can also accelerate the formation of the minor α phase as well as the major α’ phase. Full article

(This article belongs to the Special Issue Biobased Polymers)

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Review

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24 pages, 1727 KiB

Open AccessReview

Environmental Impact of Food Packaging Materials: A Review of Contemporary Development from Conventional Plastics to Polylactic Acid Based Materials

by Lindani Koketso Ncube, Albert Uchenna Ude, Enoch Nifise Ogunmuyiwa, Rozli Zulkifli and Isaac Nongwe Beas

Materials 2020, 13(21), 4994; https://doi.org/10.3390/ma13214994 - 6 Nov 2020

Cited by 244 | Viewed by 28070

Abstract

Plastics have remained the material of choice, and after serving their intended purpose, a large proportion ends up in the environment where they persist for centuries. The packaging industry is the largest and growing consumer of synthetic plastics derived from fossil fuels. Food packaging plastics account for the bulk of plastic waste that are polluting the environment. Additionally, given the fact that petroleum reserves are finite and facing depletion, there is a need for the development of alternative materials that can serve the same purpose as conventional plastics. This paper reviews the function of packaging materials and highlights the future potential of the adoption of green materials. Biopolymers have emerged as promising green materials although they still have very low market uptake. Polylactic acid (PLA) has emerged as the most favoured bioplastic. However, it is limited by its high cost and some performance drawbacks. Blending with agricultural waste and natural fillers can result in green composites at low cost, low greenhouse gas emissions, and with improved performance for food packaging applications. The continent of Africa is proposed as a rich source of fibres and fillers that can be sustainably exploited to fabricate green composites in a bid to achieve a circular economy. Full article

(This article belongs to the Special Issue Biobased Polymers)

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47 pages, 3576 KiB

Open AccessReview

Bio-Based Polymer Electrolytes for Electrochemical Devices: Insight into the Ionic Conductivity Performance

by Marwah Rayung, Min Min Aung, Shah Christirani Azhar, Luqman Chuah Abdullah, Mohd Sukor Su’ait, Azizan Ahmad and Siti Nurul Ain Md Jamil

Materials 2020, 13(4), 838; https://doi.org/10.3390/ma13040838 - 12 Feb 2020

Cited by 78 | Viewed by 8547

Abstract

With the continuing efforts to explore alternatives to petrochemical-based polymers and the escalating demand to minimize environmental impact, bio-based polymers have gained a massive amount of attention over the last few decades. The potential uses of these bio-based polymers are varied, from household goods to high end and advanced applications. To some extent, they can solve the depletion and sustainability issues of conventional polymers. As such, this article reviews the trends and developments of bio-based polymers for the preparation of polymer electrolytes that are intended for use in electrochemical device applications. A range of bio-based polymers are presented by focusing on the source, the general method of preparation, and the properties of the polymer electrolyte system, specifically with reference to the ionic conductivity. Some major applications of bio-based polymer electrolytes are discussed. This review examines the past studies and future prospects of these materials in the polymer electrolyte field. Full article

(This article belongs to the Special Issue Biobased Polymers)

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