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Advanced Biopolymer-Based Nanocomposites and Hybrid Materials

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

Deadline for manuscript submissions: closed (30 November 2020) | Viewed by 30903

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Guest Editor
CICECO—Aveiro Institute of Materials, Department of Chemistry, University of Aveiro, 3810-193 Aveiro, Portugal
Interests: production and application of biogenic nanofibers (bacterial cellulose and protein fibrils); nanostructured biocomposites; bio-based materials for biomedical applications (wound healing, drug delivery and 3D-bioprinting); biocomposites and functional paper materials; chemical modification of (nano)cellulose fibers and other polysaccharides and their characterization and applications; chemistry of lignocellulosic materials (cellulose, wood, cork, etc.)
Special Issues, Collections and Topics in MDPI journals

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Guest Editor
CICECO–Aveiro Institute of Materials, Department of Chemistry, University of Aveiro, 3810-193 Aveiro, Portugal
Interests: sustainable use of biopolymers (nanocellulose, chitosan, pullulan, proteins, etc.) for the design of functional nanostructured materials for biomedical (e.g., drug delivery and wound healing) and technological (e.g., active packaging, fuel cells, and water remediation) applications
Special Issues, Collections and Topics in MDPI journals

Special Issue Information

Dear Colleagues,

The exploitation of naturally occurring polymers to engineer advanced nanocomposites and hybrid materials is the focus of increasing scientific activity, explained by the growing environmental concerns, and the interest in the peculiar features and multiple functionalities of these macromolecules. In fact, natural polymers, such as polysaccharides (e.g., cellulose, chitin, chitosan, starch, alginate, dextran, fucoidan, heparin, hyaluronan, and pullulan) and proteins (e.g., albumin, apoferritin, casein, collagen, fibrinogen, and gelatin), present a remarkable potential for the design of all kinds of materials for application in a multitude of domains, for example, in mechanics, optics, electronics, energy, environment, biology, and medicine.

This Special Issue will collect the work of world-leading scientists on the current developments in the field of multifunctional bio-based nanocomposites and hybrid materials with a particular emphasis on their production methodologies, properties, and prominent applications. Thus, any material related to biopolymer-based nanocomposite and hybrid materials manufactured with a plethora of partners, including (but not confined to) natural polymers, bioactive compounds, and inorganic nanoparticles, is more than welcome for the Special Issue “Advanced Biopolymer-Based Nanocomposites and Hybrid Materials”.

Prof. Armando J. D. Silvestre
Dr. Carmen S. R. Freire
Prof. Dr. Carla Vilela
Guest Editors

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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. Materials is an international peer-reviewed open access semimonthly journal published by MDPI.

Please visit the Instructions for Authors page before submitting a manuscript. The Article Processing Charge (APC) for publication in this open access journal is 2600 CHF (Swiss Francs). 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

  • Biopolymers
  • polysaccharides
  • proteins
  • nanocomposites
  • hybrids
  • aerogels
  • films
  • fibers
  • biomedical applications
  • technological applications

Published Papers (7 papers)

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Editorial

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2 pages, 177 KiB  
Editorial
Special Issue: Advanced Biopolymer-Based Nanocomposites and Hybrid Materials
by Armando J. D. Silvestre, Carmen S. R. Freire and Carla Vilela
Materials 2021, 14(3), 493; https://0-doi-org.brum.beds.ac.uk/10.3390/ma14030493 - 21 Jan 2021
Cited by 4 | Viewed by 1610
Abstract
The gamut of natural polymers, from polysaccharides to proteins, exhibit peculiar features and multiple functionalities that are being exploited to engineer advanced nanocomposites and hybrid materials [...] Full article
(This article belongs to the Special Issue Advanced Biopolymer-Based Nanocomposites and Hybrid Materials)

Research

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18 pages, 4916 KiB  
Article
Roles of Silk Fibroin on Characteristics of Hyaluronic Acid/Silk Fibroin Hydrogels for Tissue Engineering of Nucleus Pulposus
by Tze-Wen Chung, Weng-Pin Chen, Pei-Wen Tai, Hsin-Yu Lo and Ting-Ya Wu
Materials 2020, 13(12), 2750; https://0-doi-org.brum.beds.ac.uk/10.3390/ma13122750 - 17 Jun 2020
Cited by 23 | Viewed by 4002
Abstract
Silk fibroin (SF) and hyaluronic acid (HA) were crosslinked by horseradish peroxidase (HRP)/H2O2, and 1,4-Butanediol di-glycidyl ether (BDDE), respectively, to produce HA/SF-IPN (interpenetration network) (HS-IPN) hydrogels. HS-IPN hydrogels consisted of a SF strain with a high content of tyrosine [...] Read more.
Silk fibroin (SF) and hyaluronic acid (HA) were crosslinked by horseradish peroxidase (HRP)/H2O2, and 1,4-Butanediol di-glycidyl ether (BDDE), respectively, to produce HA/SF-IPN (interpenetration network) (HS-IPN) hydrogels. HS-IPN hydrogels consisted of a SF strain with a high content of tyrosine (e.g., strain A) increased viscoelastic modules compared with those with low contents (e.g., strain B and C). Increasing the quantities of SF in HS-IPN hydrogels (e.g., HS7-IPN hydrogels with weight ratio of HA/SF, 5:7) increased viscoelastic modules of the hydrogels. In addition, the mean pores size of scaffolds of the model hydrogels were around 38.96 ± 5.05 μm which was between those of scaffolds H and S hydrogels. Since the viscoelastic modulus of the HS7-IPN hydrogel were similar to those of human nucleus pulposus (NP), it was chosen as the model hydrogel for examining the differentiation of human bone marrow-derived mesenchymal stem cell (hBMSC) to NP. The differentiation of hBMSC induced by transforming growth factor β3 (TGF-β3) in the model hydrogels to NP cells for 7 d significantly enhanced the expressions of glycosaminoglycan (GAG) and collagen type II, and gene expressions of aggrecan and collagen type II while decreased collagen type I compared with those in cultural wells. In summary, the model hydrogels consisted of SF of strain A, and high concentrations of SF showed the highest viscoelastic modulus than those of others produced in this study, and the model hydrogels promoted the differentiation of hBMSC to NP cells. Full article
(This article belongs to the Special Issue Advanced Biopolymer-Based Nanocomposites and Hybrid Materials)
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14 pages, 3476 KiB  
Article
One-Minute Synthesis of Size-Controlled Fucoidan-Gold Nanosystems: Antitumoral Activity and Dark Field Imaging
by Ricardo J. B. Pinto, Daniela Bispo, Carla Vilela, Alexandre M. P. Botas, Rute A. S. Ferreira, Ana C. Menezes, Fábio Campos, Helena Oliveira, Maria H. Abreu, Sónia A. O. Santos and Carmen S. R. Freire
Materials 2020, 13(5), 1076; https://0-doi-org.brum.beds.ac.uk/10.3390/ma13051076 - 28 Feb 2020
Cited by 12 | Viewed by 2616
Abstract
Gold nanoparticles (AuNPs) are one of the most studied nanosystems with great potential for biomedical applications, including cancer therapy. Although some gold-based systems have been described, the use of green and faster methods that allow the control of their properties is of prime [...] Read more.
Gold nanoparticles (AuNPs) are one of the most studied nanosystems with great potential for biomedical applications, including cancer therapy. Although some gold-based systems have been described, the use of green and faster methods that allow the control of their properties is of prime importance. Thus, the present study reports a one-minute microwave-assisted synthesis of fucoidan-coated AuNPs with controllable size and high antitumoral activity. The NPs were synthesized using a fucoidan-enriched fraction extracted from Fucus vesiculosus, as the reducing and capping agent. The ensuing monodispersed and spherical NPs exhibit tiny diameters between 5.8 and 13.4 nm for concentrations of fucoidan between 0.5 and 0.05% (w/v), respectively, as excellent colloidal stability in distinct solutions and culture media. Furthermore, the NPs present antitumoral activity against three human tumor cell lines (MNT-1, HepG2, and MG-63), and flow cytometry in combination with dark-field imaging confirmed the cellular uptake of NPs by MG-63 cell line. Full article
(This article belongs to the Special Issue Advanced Biopolymer-Based Nanocomposites and Hybrid Materials)
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16 pages, 2626 KiB  
Article
Biocompatibility Investigation of Hybrid Organometallic Polymers for Sub-Micron 3D Printing via Laser Two-Photon Polymerisation
by Evaldas Balčiūnas, Nadežda Dreižė, Monika Grubliauskaitė, Silvija Urnikytė, Egidijus Šimoliūnas, Virginija Bukelskienė, Mindaugas Valius, Sara J. Baldock, John G. Hardy and Daiva Baltriukienė
Materials 2019, 12(23), 3932; https://0-doi-org.brum.beds.ac.uk/10.3390/ma12233932 - 27 Nov 2019
Cited by 4 | Viewed by 2918
Abstract
Hybrid organometallic polymers are a class of functional materials which can be used to produce structures with sub-micron features via laser two-photon polymerisation. Previous studies demonstrated the relative biocompatibility of Al and Zr containing hybrid organometallic polymers in vitro. However, a deeper understanding [...] Read more.
Hybrid organometallic polymers are a class of functional materials which can be used to produce structures with sub-micron features via laser two-photon polymerisation. Previous studies demonstrated the relative biocompatibility of Al and Zr containing hybrid organometallic polymers in vitro. However, a deeper understanding of their effects on intracellular processes is needed if a tissue engineering strategy based on these materials is to be envisioned. Herein, primary rat myogenic cells were cultured on spin-coated Al and Zr containing polymer surfaces to investigate how each material affects the viability, adhesion strength, adhesion-associated protein expression, rate of cellular metabolism and collagen secretion. We found that the investigated surfaces supported cellular growth to full confluency. A subsequent MTT assay showed that glass and Zr surfaces led to higher rates of metabolism than did the Al surfaces. A viability assay revealed that all surfaces supported comparable levels of cell viability. Cellular adhesion strength assessment showed an insignificantly stronger relative adhesion after 4 h of culture than after 24 h. The largest amount of collagen was secreted by cells grown on the Al-containing surface. In conclusion, the materials were found to be biocompatible in vitro and have potential for bioengineering applications. Full article
(This article belongs to the Special Issue Advanced Biopolymer-Based Nanocomposites and Hybrid Materials)
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15 pages, 4190 KiB  
Article
Lignin: A Biopolymer from Forestry Biomass for Biocomposites and 3D Printing
by Mihaela Tanase-Opedal, Eduardo Espinosa, Alejandro Rodríguez and Gary Chinga-Carrasco
Materials 2019, 12(18), 3006; https://0-doi-org.brum.beds.ac.uk/10.3390/ma12183006 - 16 Sep 2019
Cited by 128 | Viewed by 10010
Abstract
Biopolymers from forestry biomass are promising for the sustainable development of new biobased materials. As such, lignin and fiber-based biocomposites are plausible renewable alternatives to petrochemical-based products. In this study, we have obtained lignin from Spruce biomass through a soda pulping process. The [...] Read more.
Biopolymers from forestry biomass are promising for the sustainable development of new biobased materials. As such, lignin and fiber-based biocomposites are plausible renewable alternatives to petrochemical-based products. In this study, we have obtained lignin from Spruce biomass through a soda pulping process. The lignin was used for manufacturing biocomposite filaments containing 20% and 40% lignin and using polylactic acid (PLA) as matrix material. Dogbones for mechanical testing were 3D printed by fused deposition modelling. The lignin and the corresponding biocomposites were characterized in detail, including thermo-gravimetric analysis (TGA), differential scanning calorimetry (DSC), Fourier transform infrared (FTIR) spectroscopy, X-ray diffraction analysis (XRD), antioxidant capacity, mechanical properties, and scanning electron microscopy (SEM). Although lignin led to a reduction of the tensile strength and modulus, the reduction could be counteracted to some extent by adjusting the 3D printing temperature. The results showed that lignin acted as a nucleating agent and thus led to further crystallization of PLA. The radical scavenging activity of the biocomposites increased to roughly 50% antioxidant potential/cm2, for the biocomposite containing 40 wt % lignin. The results demonstrate the potential of lignin as a component in biocomposite materials, which we show are adequate for 3D printing operations. Full article
(This article belongs to the Special Issue Advanced Biopolymer-Based Nanocomposites and Hybrid Materials)
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16 pages, 3876 KiB  
Article
Zwitterionic Nanocellulose-Based Membranes for Organic Dye Removal
by Carla Vilela, Catarina Moreirinha, Adelaide Almeida, Armando J. D. Silvestre and Carmen S. R. Freire
Materials 2019, 12(9), 1404; https://0-doi-org.brum.beds.ac.uk/10.3390/ma12091404 - 30 Apr 2019
Cited by 42 | Viewed by 3722
Abstract
The development of efficient and environmentally-friendly nanomaterials to remove contaminants and pollutants (including harmful organic dyes) ravaging water sources is of major importance. Herein, zwitterionic nanocomposite membranes consisting of cross-linked poly(2-methacryloyloxyethyl phosphorylcholine) (PMPC) and bacterial nanocellulose (BNC) were prepared and tested as tools [...] Read more.
The development of efficient and environmentally-friendly nanomaterials to remove contaminants and pollutants (including harmful organic dyes) ravaging water sources is of major importance. Herein, zwitterionic nanocomposite membranes consisting of cross-linked poly(2-methacryloyloxyethyl phosphorylcholine) (PMPC) and bacterial nanocellulose (BNC) were prepared and tested as tools for water remediation. These nanocomposite membranes fabricated via the one-pot polymerization of the zwitterionic monomer, 2-methacryloyloxyethyl phosphorylcholine, within the BNC three-dimensional porous network, exhibit thermal stability up to 250 °C, good mechanical performance (Young’s modulus ≥ 430 MPa) and high water-uptake capacity (627%–912%) in different pH media. Moreover, these zwitterionic membranes reduced the bacterial concentration of both gram-positive (Staphylococcus aureus) and gram-negative (Escherichia coli) pathogenic bacteria with maxima of 4.3– and 1.8–log CFU reduction, respectively, which might be a major advantage in reducing or avoiding bacterial growth in contaminated water. The removal of two water-soluble model dyes, namely methylene blue (MB, cationic) and methyl orange (MO, anionic), from water was also assessed and the results demonstrated that both dyes were successfully removed under the studied conditions, reaching a maximum of ionic dye adsorption of ca. 4.4–4.5 mg g−1. This combination of properties provides these PMPC/BNC nanocomposites with potential for application as antibacterial bio-based adsorbent membranes for water remediation of anionic and cationic dyes. Full article
(This article belongs to the Special Issue Advanced Biopolymer-Based Nanocomposites and Hybrid Materials)
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12 pages, 1945 KiB  
Article
Noble Metal Composite Porous Silk Fibroin Aerogel Fibers
by Alexander N. Mitropoulos, F. John Burpo, Chi K. Nguyen, Enoch A. Nagelli, Madeline Y. Ryu, Jenny Wang, R. Kenneth Sims, Kamil Woronowicz and J. Kenneth Wickiser
Materials 2019, 12(6), 894; https://0-doi-org.brum.beds.ac.uk/10.3390/ma12060894 - 18 Mar 2019
Cited by 37 | Viewed by 4836
Abstract
Nobel metal composite aerogel fibers made from flexible and porous biopolymers offer a wide range of applications, such as in catalysis and sensing, by functionalizing the nanostructure. However, producing these composite aerogels in a defined shape is challenging for many protein-based biopolymers, especially [...] Read more.
Nobel metal composite aerogel fibers made from flexible and porous biopolymers offer a wide range of applications, such as in catalysis and sensing, by functionalizing the nanostructure. However, producing these composite aerogels in a defined shape is challenging for many protein-based biopolymers, especially ones that are not fibrous proteins. Here, we present the synthesis of silk fibroin composite aerogel fibers up to 2 cm in length and a diameter of ~300 μm decorated with noble metal nanoparticles. Lyophilized silk fibroin dissolved in hexafluoro-2-propanol (HFIP) was cast in silicon tubes and physically crosslinked with ethanol to produce porous silk gels. Composite silk aerogel fibers with noble metals were created by equilibrating the gels in noble metal salt solutions reduced with sodium borohydride, followed by supercritical drying. These porous aerogel fibers provide a platform for incorporating noble metals into silk fibroin materials, while also providing a new method to produce porous silk fibers. Noble metal silk aerogel fibers can be used for biological sensing and energy storage applications. Full article
(This article belongs to the Special Issue Advanced Biopolymer-Based Nanocomposites and Hybrid Materials)
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