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Smart Biobased Polymers and Composites: Current Challenges and Opportunities

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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 (31 July 2022) | Viewed by 30197

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Special Issue Editor

Prof. Dr. Vijay Kumar Thakur

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Guest Editor

1. Biorefining and Advanced Materials Research Centre, SRUC, Edinburgh EH9 3JG, UK
2. Enhanced Composites and Structures Center, School of Aerospace, Transport and Manufacturing, Cranfield University, Cranfield MK43 0AL, UK
Interests: biorefining, chemistry, nanotechnology, biomass, and waste; biomedical engineering; composites; sensors; manufacturing of functional materials; aerospace materials; nanomaterials; renewable energy; smart materials; surface engineering; water science and engineering; additive manufacturing of polymers and composites; multifunctional polymer composites and nanocomposites: self-healing, nanoelectronic materials; hydrogels; membranes; nanofiber; composites for extreme environments and manufacturing technology
Special Issues, Collections and Topics in MDPI journals

Special Issue Information

Dear Colleagues,

The 21st century poses vast challenges for researchers all around the globe, especially regarding the effective use of sustainable polymers and their materials for different applications. With this focus, sustainable polymers and composites from biorenewable sources are now rising as one of the most feasible alternatives to traditional synthetic polymers/materials for a variety of industrial applications.

This Special Issue of IJMS will cover the most recent advancements in the bio-based polymers and respective materials. Potential topics include, but are not limited to the following:

Biorefining and biorefineries
Biopolymers
Biocomposites; natural rubber
Biobased additives for polymers
Green chemicals precursors
Multifunctional or smart biobased polymers and composites
New insights into the sustainable polymers and their applications
Natural fiber-based polymers and composites
Polymer blends from natural resources
Rational design and understanding of sustainable polymers from different biorenewable resources
Synthesis and characterization of natural fiber-derived cellulosic materials (micro/nano)

Prof. Dr. Vijay Kumar Thakur
Guest Editor

Manuscript Submission Information

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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. International Journal of Molecular Sciences is an international peer-reviewed open access semimonthly journal published by MDPI.

Please visit the Instructions for Authors page before submitting a manuscript. There is an Article Processing Charge (APC) for publication in this open access journal. For details about the APC please see here. 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

analysis and characterization of bio-based polymers and composites
biomass
biodegradable polymers matrices
biodegradability
bio-based polymers and composites
bio-based resins
eco-friendly natural polymers
novel biocomposites
synthesis of bio-based polymers
sustainable materials

Published Papers (11 papers)

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Research

Jump to: Review

15 pages, 3401 KiB

Open AccessArticle

Effect of Transglutaminase Post-Treatment on the Stability and Swelling Behavior of Casein Micro-Particles

by Ronald Gebhardt, Sahel Khanna, Jann Schulte and Md Asaduzzaman

Int. J. Mol. Sci. 2022, 23(19), 11837; https://doi.org/10.3390/ijms231911837 - 05 Oct 2022

Cited by 4 | Viewed by 1905

Abstract

Casein microparticles are produced by flocculation of casein micelles due to volume exclusion of pectin and subsequent stabilization by film drying. Transglutaminase post-treatment alters their stability, swelling behavior, and internal structure. Untreated particles sediment due to their size and disintegrate completely after the addition of sodium dodecyl sulfate. The fact that transglutaminase-treated microparticles only sediment at comparable rates under these conditions shows that their structural integrity is not lost due to the detergent. Transglutaminase-treated particles reach an equilibrium final size after swelling instead of decomposing completely. By choosing long treatment times, swelling can also be completely suppressed as experiments at pH 11 show. In addition, deswelling effects also occur within the swelling curves, which enhance with increasing transglutaminase treatment time and are ascribed to the elastic network of cross-linked caseins. We propose a structural model for transglutaminase-treated microparticles consisting of a core of uncross-linked and a shell of cross-linked caseins. A dynamic model describes all swelling curves by considering both casein fractions in parallel. The characteristic correlation length of the internal structure of swollen casein microparticles is pH-independent and decreases with increasing transglutaminase treatment time, as observed also for the equilibrium swelling value of uncross-linked caseins. Full article

(This article belongs to the Special Issue Smart Biobased Polymers and Composites: Current Challenges and Opportunities)

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24 pages, 18870 KiB

Open AccessArticle

Formulation of Magneto-Responsive Hydrogels from Dually Cross-Linked Polysaccharides: Synthesis, Tuning and Evaluation of Rheological Properties

by Lenka Vítková, Lenka Musilová, Eva Achbergerová, Roman Kolařík, Miroslav Mrlík, Kateřina Korpasová, Leona Mahelová, Zdenka Capáková and Aleš Mráček

Int. J. Mol. Sci. 2022, 23(17), 9633; https://doi.org/10.3390/ijms23179633 - 25 Aug 2022

Cited by 7 | Viewed by 1802

Abstract

Smart hydrogels based on natural polymers present an opportunity to fabricate responsive scaffolds that provide an immediate and reversible reaction to a given stimulus. Modulation of mechanical characteristics is especially interesting in myocyte cultivation, and can be achieved by magnetically controlled stiffening. Here, hyaluronan hydrogels with carbonyl iron particles as a magnetic filler are prepared in a low-toxicity process. Desired mechanical behaviour is achieved using a combination of two cross-linking routes—dynamic Schiff base linkages and ionic cross-linking. We found that gelation time is greatly affected by polymer chain conformation. This factor can surpass the influence of the number of reactive sites, shortening gelation from 5 h to 20 min. Ionic cross-linking efficiency increased with the number of carboxyl groups and led to the storage modulus reaching 10

^{3}

Pa compared to 10

^{1}

Pa–10

^{2}

Pa for gels cross-linked with only Schiff bases. Furthermore, the ability of magnetic particles to induce significant stiffening of the hydrogel through the magnetorheological effect is confirmed, as a 10

^{3}

-times higher storage modulus is achieved in an external magnetic field of 842 kA·m

^{- 1}

. Finally, cytotoxicity testing confirms the ability to produce hydrogels that provide over 75% relative cell viability. Therefore, dual cross-linked hyaluronan-based magneto-responsive hydrogels present a potential material for on-demand mechanically tunable scaffolds usable in myocyte cultivation. Full article

(This article belongs to the Special Issue Smart Biobased Polymers and Composites: Current Challenges and Opportunities)

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17 pages, 4497 KiB

Open AccessArticle

Maleic Anhydride-Grafted PLA Preparation and Characteristics of Compatibilized PLA/PBSeT Blend Films

by Hyunho Jang, Sangwoo Kwon, Sun Jong Kim and Su-il Park

Int. J. Mol. Sci. 2022, 23(13), 7166; https://doi.org/10.3390/ijms23137166 - 28 Jun 2022

Cited by 10 | Viewed by 2825

Abstract

Poly(butylene sebacate-co-terephthalate) (PBSeT) is a biodegradable flexible polymer suitable for melt blending with other biodegradable polymers. Melt blending with a compatibilizer is a common strategy for increasing miscibility between polymers. In this study, PBSeT polyester was synthesized, and poly(lactic acid) (PLA) was blended with 25 wt% PBSeT by melt processing with 3–6 phr PLA-grafted maleic anhydride (PLA-g-MAH) compatibilizers. PLA-g-MAH enhanced the interfacial adhesion of the PLA/PBSeT blend, and their mechanical and morphological properties confirmed that the miscibility also increased. Adding more than 6 phr of PLA-g-MAH significantly improved the mechanical properties and accelerated the cold crystallization of the PLA/PBSeT blends. Furthermore, the thermal stabilities of the blends with PLA-g-MAH were slightly enhanced. PLA/PBSeT blends with and without PLA-g-MAH were not significantly different after 120 h, whereas all blends showed a more facilitated hydrolytic degradation rate than neat PLA. These findings indicate that PLA-g-MAH effectively improves PLA/PBSeT compatibility and can be applied in the packaging industry. Full article

(This article belongs to the Special Issue Smart Biobased Polymers and Composites: Current Challenges and Opportunities)

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13 pages, 2435 KiB

Open AccessArticle

A Novel Method of Endotoxins Removal from Chitosan Hydrogel as a Potential Bioink Component Obtained by CO₂ Saturation

by Adrianna Banach-Kopeć, Szymon Mania, Joanna Pilch, Ewa Augustin, Iwona Gabriel and Robert Tylingo

Int. J. Mol. Sci. 2022, 23(10), 5505; https://doi.org/10.3390/ijms23105505 - 14 May 2022

Cited by 3 | Viewed by 2094

Abstract

The article presents a new approach in the purification of chitosan (CS) hydrogel in order to remove a significant amount of endotoxins without changing its molecular weight and viscosity. Two variants of the method used to purify CS hydrogels from endotoxins were investigated using the PyroGene rFC Enzymatic Cascade assay kit. The effect of the CS purification method was assessed in terms of changes in the dynamic viscosity of its hydrogels, the molecular weight of the polymer, microbiological purity after refrigerated storage and cytotoxicity against L929 cells based on the ISO 10993-5:2009(E) standard. The proposed purification method 1 (M1) allows for the removal of significant amounts of endotoxins: 87.9–97.6% in relation to their initial concentration in the CS hydrogel without affecting the solution viscosity. Moreover, the final solutions were sterile and microbiologically stable during storage. The M1 purification method did not change the morphology of the L929 cells. Full article

(This article belongs to the Special Issue Smart Biobased Polymers and Composites: Current Challenges and Opportunities)

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15 pages, 7623 KiB

Open AccessArticle

Treatment of Critical Size Femoral Bone Defects with Biomimetic Hybrid Scaffolds of 3D Plotted Calcium Phosphate Cement and Mineralized Collagen Matrix

by Anna Carla Culla, Corina Vater, Xinggui Tian, Julia Bolte, Tilman Ahlfeld, Henriette Bretschneider, Alexander Pape, Stuart B. Goodman, Michael Gelinsky and Stefan Zwingenberger

Int. J. Mol. Sci. 2022, 23(6), 3400; https://doi.org/10.3390/ijms23063400 - 21 Mar 2022

Cited by 5 | Viewed by 3304

Abstract

To treat critical-size bone defects, composite materials and tissue-engineered bone grafts play important roles in bone repair materials. The purpose of this study was to investigate the bone regenerative potential of hybrid scaffolds consisting of macroporous calcium phosphate cement (CPC) and microporous mineralized collagen matrix (MCM). Hybrid scaffolds were synthetized by 3D plotting CPC and then filling with MCM (MCM-CPC group) and implanted into a 5 mm critical size femoral defect in rats. Defects left empty (control group) as well as defects treated with scaffolds made of CPC only (CPC group) and MCM only (MCM group) served as controls. Eight weeks after surgery, micro-computed tomography scans and histological analysis were performed to analyze the newly formed bone, the degree of defect healing and the activity of osteoclasts. Mechanical stability was tested by 3-point-bending of the explanted femora. Compared with the other groups, more newly formed bone was found within MCM-CPC scaffolds. The new bone tissue had a clamp-like structure which was fully connected to the hybrid scaffolds and thereby enhanced the biomechanical strength. Together, the biomimetic hybrid MCM-CPC scaffolds enhanced bone defect healing by improved osseointegration and their differentiated degradation provides spatial effects in the process of critical-bone defect healing. Full article

(This article belongs to the Special Issue Smart Biobased Polymers and Composites: Current Challenges and Opportunities)

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23 pages, 9774 KiB

Open AccessArticle

Characterization of a Novel Aspect of Tissue Scarring Following Experimental Spinal Cord Injury and the Implantation of Bioengineered Type-I Collagen Scaffolds in the Adult Rat: Involvement of Perineurial-like Cells?

by Haktan Altinova, Pascal Achenbach, Moniek Palm, Istvan Katona, Emmanuel Hermans, Hans Clusmann, Joachim Weis and Gary Anthony Brook

Int. J. Mol. Sci. 2022, 23(6), 3221; https://doi.org/10.3390/ijms23063221 - 16 Mar 2022

Cited by 1 | Viewed by 2187

Abstract

Numerous intervention strategies have been developed to promote functional tissue repair following experimental spinal cord injury (SCI), including the bridging of lesion-induced cystic cavities with bioengineered scaffolds. Integration between such implanted scaffolds and the lesioned host spinal cord is critical for supporting regenerative growth, but only moderate-to-low degrees of success have been reported. Light and electron microscopy were employed to better characterise the fibroadhesive scarring process taking place after implantation of a longitudinally microstructured type-I collagen scaffold into unilateral mid-cervical resection injuries of the adult rat spinal cord. At long survival times (10 weeks post-surgery), sheets of tightly packed cells (of uniform morphology) could be seen lining the inner surface of the repaired dura mater of lesion-only control animals, as well as forming a barrier along the implant–host interface of the scaffold-implanted animals. The highly uniform ultrastructural features of these scarring cells and their anatomical continuity with the local, reactive spinal nerve roots strongly suggest their identity to be perineurial-like cells. This novel aspect of the cellular composition of reactive spinal cord tissue highlights the increasingly complex nature of fibroadhesive scarring involved in traumatic injury, and particularly in response to the implantation of bioengineered collagen scaffolds. Full article

(This article belongs to the Special Issue Smart Biobased Polymers and Composites: Current Challenges and Opportunities)

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25 pages, 4946 KiB

Open AccessArticle

Cyprinus carpio Skeleton Byproduct as a Source of Collagen for Gelatin Preparation

by Robert Gál, Pavel Mokrejš, Jana Pavlačková and Dagmar Janáčová

Int. J. Mol. Sci. 2022, 23(6), 3164; https://doi.org/10.3390/ijms23063164 - 15 Mar 2022

Cited by 1 | Viewed by 2434

Abstract

Byproducts obtained from fish processing account for up to 70% of their live weight and represent a large amount of unused raw materials rich in proteins, fats, minerals, and vitamins. Recently, the management of the use of predominantly cold-water fish byproducts has become a priority for many processing companies. This paper describes the biotechnological processing of byproducts of warm-water Cyprinus carpio skeletons into gelatins. A Taguchi experimental design with two process factors (HCl concentration during demineralization of the starting material and the amount of enzyme during enzyme conditioning of the collagen) examined at three levels (0.5, 1.0 and 2.0 wt%; 0.0, 0.1 and 0.2 wt% respectively) was used to optimize the processing of fish tissue into gelatin. Depending on the preparation conditions, four gelatin fractions were prepared by multi-stage extraction from the starting material with a total yield of 18.7–55.7%. Extensive characterization of the gel-forming and surface properties of the prepared gelatins was performed. Gelatins belong to the group of zero–low-medium Bloom value (0–170 Bloom) and low–medium viscosity (1.1–4.9 mPa·s) gelatins and are suitable for some food, pharmaceutical, and cosmetic applications. During processing, the pigment can be isolated; the remaining solid product can then be used in agriculture, and H₃PO₄Ca can be precipitated from the liquid byproduct after demineralization. The carp byproduct processing technology is environmentally friendly and meets the requirements of zero-waste technology. Full article

(This article belongs to the Special Issue Smart Biobased Polymers and Composites: Current Challenges and Opportunities)

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17 pages, 1941 KiB

Open AccessArticle

Oxidation of Various Kraft Lignins with a Bacterial Laccase Enzyme

by Sebastian A. Mayr, Raditya Subagia, Renate Weiss, Nikolaus Schwaiger, Hedda K. Weber, Johannes Leitner, Doris Ribitsch, Gibson S. Nyanhongo and Georg M. Guebitz

Int. J. Mol. Sci. 2021, 22(23), 13161; https://doi.org/10.3390/ijms222313161 - 06 Dec 2021

Cited by 12 | Viewed by 3348

Abstract

Modification of kraft lignin (KL), traditionally uses harsh and energy-demanding physical and chemical processes. In this study, the potential of the bacterial laccase CotA (spore coating protein A) for oxidation of KL under mild conditions was assessed. Thereby, the efficiency of CotA to oxidize both softwood and hardwood KL of varying purity at alkaline conditions was examined. For the respective type of wood, the highest oxidation activity by CotA was determined for the medium ash content softwood KL (MA_S) and the medium ash content hardwood KL (MA_H), respectively. By an up to 95% decrease in fluorescence and up to 65% in phenol content coupling of the structural lignin units was indicated. These results correlated with an increase in viscosity and molecular weight, which increased nearly 2 and 20-fold for MA_H and about 1.3 and 6.0-fold for MA_S, respectively. Thus, this study confirms that the CotA laccase can oxidize a variety of KL at alkaline conditions, while the origin and purity of KL were found to have a major impact on the efficiency of oxidation. Under the herein tested conditions, it was observed that the MA_H KL showed the highest susceptibility to CotA oxidation when compared to the other hardwood KLs and the softwood KLs. Therefore, this could be a viable method to produce sustainable resins and adhesives. Full article

(This article belongs to the Special Issue Smart Biobased Polymers and Composites: Current Challenges and Opportunities)

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22 pages, 7477 KiB

Open AccessArticle

Lignin and Xylan as Interface Engineering Additives for Improved Environmental Durability of Sustainable Cellulose Nanopapers

by Sergejs Beluns, Oskars Platnieks, Sergejs Gaidukovs, Olesja Starkova, Alisa Sabalina, Liga Grase, Vijay Kumar Thakur and Gerda Gaidukova

Int. J. Mol. Sci. 2021, 22(23), 12939; https://doi.org/10.3390/ijms222312939 - 29 Nov 2021

Cited by 18 | Viewed by 2754

Abstract

Cellulose materials and products are frequently affected by environmental factors such as light, temperature, and humidity. Simulated UV irradiation, heat, and moisture exposure were comprehensively used to characterize changes in cellulose nanopaper (NP) tensile properties. For the preparation of NP, high-purity cellulose from old, unused filter paper waste was used. Lignin and xylan were used as sustainable green interface engineering modifiers for NP due to their structural compatibility, low price, nontoxic nature, and abundance as a by-product of biomass processing, as well as their ability to protect cellulose fibers from UV irradiation. Nanofibrillated cellulose (NFC) suspension was obtained by microfluidizing cellulose suspension, and NP was produced by casting films from water suspensions. The use of filler from 1 to 30 wt% significantly altered NP properties. All nanopapers were tested for their sensitivity to water humidity, which reduced mechanical properties from 10 to 40% depending on the saturation level. Xylan addition showed a significant increase in the specific elastic modulus and specific strength by 1.4- and 2.8-fold, respectively. Xylan-containing NPs had remarkable resistance to UV irradiation, retaining 50 to 90% of their initial properties. Lignin-modified NPs resulted in a decreased mechanical performance due to the particle structure of the filler and the agglomeration process, but it was compensated by good property retention and enhanced elongation. The UV oxidation process of the NP interface was studied with UV-Vis and FTIR spectroscopy, which showed that the degradation of lignin and xylan preserves a cellulose fiber structure. Scanning electron microscopy images revealed the structural formation of the interface and supplemented understanding of UV aging impact on the surface and penetration depth in the cross-section. The ability to overcome premature aging in environmental factors can significantly benefit the wide adaption of NP in food packaging and functional applications. Full article

(This article belongs to the Special Issue Smart Biobased Polymers and Composites: Current Challenges and Opportunities)

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19 pages, 5557 KiB

Open AccessArticle

A Comparison Study on the Magneto-Responsive Properties and Swelling Behaviors of a Polyacrylamide-Based Hydrogel Incorporating with Magnetic Particles

by Chanchan Xu, Bin Li and Xiaojie Wang

Int. J. Mol. Sci. 2021, 22(22), 12342; https://doi.org/10.3390/ijms222212342 - 15 Nov 2021

Cited by 3 | Viewed by 1888

Abstract

This work investigates the mechanical properties, microstructures, and water-swelling behavior of a novel hydrogel filled with magnetic particles. The nanoparticles of magnetite (Fe₃O₄) and the micro-particles of carbonyl iron (CI) were selected and filled into a polyacrylamide (PAAM) hydrogel matrix to create two types of magnetic hydrogels. The isotropy and anisotropy of magnetic hydrogels are also presented in this study. The isotropic samples were cured without applying a magnetic field (MF), and the anisotropic samples were cured by applying an MF in the direction perpendicular to the thickness of the samples. The effects of the size, content, and inner structures of magnetic particles on the magneto-responsive and swelling properties of magnetic hydrogels were investigated. It was found that the magnetorheological (MR) effect of anisotropic samples was apparently higher than that of isotropic samples, and the hydrogels with CI exhibited a noticeable MR effect than those with Fe₃O₄. The storage modulus can be enhanced by increasing the filler content and size, forming an anisotropic structure, and applying an external MF. In addition, the magnetic hydrogels also have a swelling ability that can be tuned by varying the content and size of the particle fillers. Full article

(This article belongs to the Special Issue Smart Biobased Polymers and Composites: Current Challenges and Opportunities)

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Review

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29 pages, 5964 KiB

Open AccessReview

Magnetic Fluorescent Quantum Dots Nanocomposites in Food Contaminants Analysis: Current Challenges and Opportunities

by Jincheng Xiong, Huixia Zhang, Linqian Qin, Shuai Zhang, Jiyue Cao and Haiyang Jiang

Int. J. Mol. Sci. 2022, 23(8), 4088; https://doi.org/10.3390/ijms23084088 - 07 Apr 2022

Cited by 16 | Viewed by 3044

Abstract

The presence of food contaminants can cause foodborne illnesses, posing a severe threat to human health. Therefore, a rapid, sensitive, and convenient method for monitoring food contaminants is eagerly needed. The complex matrix interferences of food samples and poor performance of existing sensing probes bring significant challenges to improving detection performances. Nanocomposites with multifunctional features provide a solution to these problems. The combination of the superior characteristics of magnetic nanoparticles (MNPs) and quantum dots (QDs) to fabricate magnetic fluorescent quantum dots (MNPs@QDs) nanocomposites are regarded as an ideal multifunctional probe for food contaminants analysis. The high-efficiency pretreatment and rapid fluorescence detection are concurrently integrated into one sensing platform using MNPs@QDs nanocomposites. In this review, the contemporary synthetic strategies to fabricate MNPs@QDs, including hetero-crystalline growth, template embedding, layer-by-layer assembly, microemulsion technique, and one-pot method, are described in detail, and their advantages and limitations are discussed. The recent advances of MNPs@QDs nanocomposites in detecting metal ions, foodborne pathogens, toxins, pesticides, antibiotics, and illegal additives are comprehensively introduced from the perspectives of modes and detection performances. The review ends with current challenges and opportunities in practical applications and prospects in food contaminants analysis, aiming to promote the enthusiasm for multifunctional sensing platform research. Full article

(This article belongs to the Special Issue Smart Biobased Polymers and Composites: Current Challenges and Opportunities)

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