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Functional Chitosan-Based Composites

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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 (30 September 2020) | Viewed by 42022

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Dr. Luminita Marin

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“Petru Poni” Institute of Macromolecular Chemistry, Gr. Ghica Voda Alley, 41A, 700487 Iasi, Romania
Interests: hydrogels; imine; chitosan; Schiff base; phenothiazine; azomethine; drug delivery
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Dr. Maria Bardosova

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Tyndall National Institute, Lee Maltings, Dyke Parade, Cork, Ireland
Interests: chitosan; hybrid materials; photonic crystals; sensors; thin organic films; Langmuir-Blodgett technique
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Dear Colleagues,

Technological development has been one of the defining factors of our contemporary world. Unfortunately, sometimes new technologies seem to be accompanied by dramatic side effects on both the environment and human health. Limiting such hazards is an active area of research, and the use of renewable resources for a variety of materials applications is now a major consideration in terms of hazard mitigation.

Chitosan is a sustainable biopolymer prepared from the renewable resource chitin. Among the various biopolymers known, it stands out because of its wide array of beneficial properties which prompt its use in many different applications. For example, it is non-toxic, biocompatible, biodegradable, consumer-safe and often displays superior material and functional properties as compared to other biopolymers. It can be used for the preparation of a large variety of materials types, such as hydrogels, fibres, nanostructures and films and coatings, which can then be further applied in diverse fields such as medicine, food packaging, environmental protection, cosmetics, agriculture, textiles, paper industry and so on.

The aim of this Special Issue is to present the latest developments in the field of chitosan biomaterials and their current or potential applications in, but not limited to, the areas mentioned above.

Dr. Luminita Marin
Dr. Maria Bardosova
Guest Editors

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Keywords

chitosan
hydrogels
films
coatings
fibres
nanostructures
formulations

Published Papers (11 papers)

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Research

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14 pages, 1559 KiB

Open AccessArticle

Chitosan-ZnO Nanocomposites Assessed by Dielectric, Mechanical, and Piezoelectric Properties

by Evgen Prokhorov, Gabriel Luna-Bárcenas, José Martín Yáñez Limón, Alejandro Gómez Sánchez and Yuriy Kovalenko

Polymers 2020, 12(9), 1991; https://doi.org/10.3390/polym12091991 - 01 Sep 2020

Cited by 24 | Viewed by 3917

Abstract

The aim of this work is to structurally characterize chitosan-zinc oxide nanoparticles (CS-ZnO NPs) films in a wide range of NPs concentration (0–20 wt.%). Dielectric, conductivity, mechanical, and piezoelectric properties are assessed by using thermogravimetry, FTIR, XRD, mechanical, and dielectric spectroscopy measurements. These analyses reveal that the dielectric constant, Young’s modulus, and piezoelectric constant (d₃₃) exhibit a strong dependence on nanoparticle concentration such that maximum values of referred properties are obtained at 15 wt.% of ZnO NPs. The piezoelectric coefficient d₃₃ in CS-ZnO nanocomposite films with 15 wt.% of NPs (d₃₃ = 65.9 pC/N) is higher than most of polymer-ZnO nanocomposites because of the synergistic effect of piezoelectricity of NPs, elastic properties of CS, and optimum NPs concentration. A three-phase model is used to include the chitosan matrix, ZnO NPs, and interfacial layer with dielectric constant higher than that of neat chitosan and ZnO. This layer between nanoparticles and matrix is due to strong interactions between chitosan’s side groups with ZnO NPs. The understanding of nanoscale properties of CS-ZnO nanocomposites is important in the development of biocompatible sensors, actuators, nanogenerators for flexible electronics and biomedical applications. Full article

(This article belongs to the Special Issue Functional Chitosan-Based Composites)

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24 pages, 3432 KiB

Open AccessArticle

Increased Cytotoxic Efficacy of Protocatechuic Acid in A549 Human Lung Cancer Delivered via Hydrophobically Modified-Chitosan Nanoparticles As an Anticancer Modality

by Cha Yee Kuen, Tieo Galen, Sharida Fakurazi, Siti Sarah Othman and Mas Jaffri Masarudin

Polymers 2020, 12(9), 1951; https://doi.org/10.3390/polym12091951 - 28 Aug 2020

Cited by 22 | Viewed by 3362

Abstract

The growing incidence of global lung cancer cases against successful treatment modalities has increased the demand for the development of innovative strategies to complement conventional chemotherapy, radiation, and surgery. The substitution of chemotherapeutics by naturally occurring phenolic compounds has been touted as a promising research endeavor, as they sideline the side effects of current chemotherapy drugs. However, the therapeutic efficacy of these compounds is conventionally lower than that of chemotherapeutic agents due to their lower solubility and consequently poor intracellular uptake. Therefore, we report herein a hydrophobically modified chitosan nanoparticle (pCNP) system for the encapsulation of protocatechuic acid (PCA), a naturally occurring but poorly soluble phenolic compound, for increased efficacy and improved intracellular uptake in A549 lung cancer cells. The pCNP system was modified by the inclusion of a palmitoyl group and physico-chemically characterized to assess its particle size, Polydispersity Index (PDI) value, amine group quantification, functional group profiling, and morphological properties. The inclusion of hydrophobic palmitoyl in pCNP-PCA was found to increase the encapsulation of PCA by 54.5% compared to unmodified CNP-PCA samples whilst it only conferred a 23.4% larger particle size. The single-spherical like particles with uniformed dispersity pCNP-PCA exhibited IR bands, suggesting the successful incorporation of PCA within its core, and a hydrophobic layer was elucidated via electron micrographs. The cytotoxic efficacy was then assessed by using an MTT cytotoxicity assay towards A549 human lung cancer cell line and was compared with traditional chitosan nanoparticle system. Fascinatingly, a controlled release delivery and enhanced therapeutic efficacy were observed in pCNP-PCA compared to CNP, which is ascribed to lower IC₅₀ values in the 72-h treatment in the pCNP system. Using the hydrophobic system, efficacy of PCA was significantly increased in 24-, 48-, and 72-h treatments compared to a single administration of the compound, and via the unmodified CNP system. Findings arising from this study exhibit the potential of using such modified nanoparticulate systems in increasing the efficacy of natural phenolic compounds by augmenting their delivery potential for better anti-cancer responses. Full article

(This article belongs to the Special Issue Functional Chitosan-Based Composites)

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14 pages, 3139 KiB

Open AccessArticle

Developed Chitosan/Oregano Essential Oil Biocomposite Packaging Film Enhanced by Cellulose Nanofibril

by Shunli Chen, Min Wu, Caixia Wang, Shun Yan, Peng Lu and Shuangfei Wang

Polymers 2020, 12(8), 1780; https://doi.org/10.3390/polym12081780 - 09 Aug 2020

Cited by 35 | Viewed by 4133

Abstract

The use of advanced and eco-friendly materials has become a trend in the field of food packaging. Cellulose nanofibrils (CNFs) were prepared from bleached bagasse pulp board by a mechanical grinding method and were used to enhance the properties of a chitosan/oregano essential oil (OEO) biocomposite packaging film. The growth inhibition rate of the developed films with 2% (w/w) OEO against E. coli and L. monocytogenes reached 99%. With the increased levels of added CNFs, the fibrous network structure of the films became more obvious, as was determined by SEM and the formation of strong hydrogen bonds between CNFs and chitosan was observed in FTIR spectra, while the XRD pattern suggested that the strength of diffraction peaks and crystallinity of the films slightly increased. The addition of 20% CNFs contributed to an oxygen-transmission rate reduction of 5.96 cc/m²·day and water vapor transmission rate reduction of 741.49 g/m²·day. However, the increase in CNFs contents did not significantly improve the barrier properties of the film. The addition of 60% CNFs significantly improved the barrier properties of the film to light and exhibited the lowest light transmittance (28.53%) at 600 nm. Addition of CNFs to the chitosan/OEO film significantly improved tensile strength and the addition of 60% CNFs contributed to an increase of 16.80 MPa in tensile strength. The developed chitosan/oregano essential oil/CNFs biocomposite film with favorable properties and antibacterial activity can be used as a green, functional material in the food-packaging field. It has the potential to improve food quality and extend food shelf life. Full article

(This article belongs to the Special Issue Functional Chitosan-Based Composites)

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14 pages, 5393 KiB

Open AccessArticle

Nanostructured Chitosan/Maghemite Composites Thin Film for Potential Optical Detection of Mercury Ion by Surface Plasmon Resonance Investigation

by Nurul Illya Muhamad Fauzi, Yap Wing Fen, Nur Alia Sheh Omar, Silvan Saleviter, Wan Mohd Ebtisyam Mustaqim Mohd Daniyal, Hazwani Suhaila Hashim and Mohd Nasrullah

Polymers 2020, 12(7), 1497; https://doi.org/10.3390/polym12071497 - 04 Jul 2020

Cited by 48 | Viewed by 3830

Abstract

In this study, synthesis and characterization of chitosan/maghemite (Cs/Fe₂O₃) composites thin film has been described. Its properties were characterized using Fourier transform infrared spectroscopy (FTIR), atomic force microscopy (AFM) and ultraviolet-visible spectroscopy (UV-Vis). FTIR confirmed the existence of Fe–O bond, C–N bond, C–C bond, C–O bond, O=C=O bond and O–H bond in Cs/Fe₂O₃ thin film. The surface morphology of the thin film indicated the relatively smooth and homogenous thin film, and also confirmed the interaction of Fe₂O₃ with the chitosan. Next, the UV-Vis result showed high absorbance value with an optical band gap of 4.013 eV. The incorporation of this Cs/Fe₂O₃ thin film with an optical-based method, i.e., surface plasmon resonance spectroscopy showed positive response where mercury ion (Hg²⁺) can be detected down to 0.01 ppm (49.9 nM). These results validate the potential of Cs/Fe₂O₃ thin film for optical sensing applications in Hg²⁺ detection. Full article

(This article belongs to the Special Issue Functional Chitosan-Based Composites)

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20 pages, 5652 KiB

Open AccessArticle

Design and Preparation of New Multifunctional Hydrogels Based on Chitosan/Acrylic Polymers for Drug Delivery and Wound Dressing Applications

by Ioana A. Duceac, Liliana Verestiuc, Cristina D. Dimitriu, Vasilica Maier and Sergiu Coseri

Polymers 2020, 12(7), 1473; https://doi.org/10.3390/polym12071473 - 30 Jun 2020

Cited by 41 | Viewed by 3795

Abstract

The dynamic evolution of materials with medical applications, particularly for drug delivery and wound dressing applications, gives impetus to design new proposed materials, among which, hydrogels represent a promising, powerful tool. In this context, multifunctional hydrogels have been obtained from chemically modified chitosan and acrylic polymers as cross-linkers, followed by subsequent conjugation with arginine. The hydrogels were finely tuned considering the variation of the synthetic monomer and the preparation conditions. The advantage of using both natural and synthetic polymers allowed porous networks with superabsorbent behavior, associated with a non-Fickian swelling mechanism. The in vitro release profiles for ibuprofen and the corresponding kinetics were studied, and the results revealed a swelling-controlled release. The biodegradability studies in the presence of lysozyme, along with the hemostatic evaluation and the induced fibroblast and stem cell proliferation, have shown that the prepared hydrogels exhibit characteristics that make them suitable for local drug delivery and wound dressing. Full article

(This article belongs to the Special Issue Functional Chitosan-Based Composites)

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14 pages, 1843 KiB

Open AccessArticle

Antioxidant and Moisturizing Properties of Carboxymethyl Chitosan with Different Molecular Weights

by Nareekan Chaiwong, Pimporn Leelapornpisid, Kittisak Jantanasakulwong, Pornchai Rachtanapun, Phisit Seesuriyachan, Vinyoo Sakdatorn, Noppol Leksawasdi and Yuthana Phimolsiripol

Polymers 2020, 12(7), 1445; https://doi.org/10.3390/polym12071445 - 28 Jun 2020

Cited by 53 | Viewed by 4938

Abstract

This research aimed to synthesize carboxymethyl chitosan (CMCH) from different molecular weights of chitosan including low MW (L, 50–190 kDa), medium MW (M, 210–300 kDa) and high MW (H, 310–375 kDa) on the antioxidant and moisturizing properties. The L-CMCH, M-CMCH and H-CMCH improved the water solubility by about 96%, 90% and 89%, respectively when compared to native chitosan. Higher MW resulted in more viscous of CMCH. For antioxidant properties, IC₅₀ values of DPPH and ABTS radical scavenging activity for L-CMCH were 1.70 and 1.37 mg/mL, respectively. The L-CMCH had higher antioxidant properties by DPPH and ABTS radical scavenging assay and FRAP. The moisturizing properties on pig skin using a Corneometer^® showed that 0.5% H-CMCH significantly presented (p ≤ 0.05) greater moisturizing effect than that of untreated-skin, distilled water, propylene glycol and pure chitosan from three molecular weights. Full article

(This article belongs to the Special Issue Functional Chitosan-Based Composites)

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13 pages, 4065 KiB

Open AccessArticle

A Theoretical Multifractal Model for Assessing Urea Release from Chitosan Based Formulations

by Manuela Maria Iftime, Stefan Andrei Irimiciuc, Maricel Agop, Marian Angheloiu, Lacramioara Ochiuz and Decebal Vasincu

Polymers 2020, 12(6), 1264; https://doi.org/10.3390/polym12061264 - 01 Jun 2020

Cited by 6 | Viewed by 1871

Abstract

This paper reports the calibration of a theoretical multifractal model based on empirical data on the urea release from a series of soil conditioner systems. To do this, a series of formulations was prepared by in situ hydrogelation of chitosan with salicylaldehyde in the presence of different urea amounts. The formulations were morphologically characterized by scanning electron microscopy and polarized light microscopy. The in vitro urea release was investigated in an environmentally simulated medium. The release data were fitted on five different mathematical models, Korsmeyer–Peppas, Zero order, First order, Higuchi and Hixson–Crowell, which allowed the establishment of a mechanism of urea release. Furthermore, a multifractal model, used for the fertilizer release for the first time, was calibrated using these empirical data. The resulting fit was in good agreement with the experimental data, validating the multifractal theoretical model. Full article

(This article belongs to the Special Issue Functional Chitosan-Based Composites)

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18 pages, 4852 KiB

Open AccessFeature PaperArticle

Development and Performance of Bioactive Compounds-Loaded Cellulose/Collagen/Polyurethane Materials

by Iuliana Spiridon, Narcis Anghel, Maria Valentina Dinu, Stelian Vlad, Adrian Bele, Bianca Iulia Ciubotaru, Liliana Verestiuc and Daniela Pamfil

Polymers 2020, 12(5), 1191; https://doi.org/10.3390/polym12051191 - 23 May 2020

Cited by 26 | Viewed by 3188

Abstract

Here we present a new biomaterial based on cellulose, collagen and polyurethane, obtained by dissolving in butyl imidazole chloride. This material served as a matrix for the incorporation of tannin and lipoic acid, as well as bioactive substances with antioxidant properties. The introduction of these bioactive principles into the base matrix led to an increase of the compressive strength in the range 105–139 kPa. An increase of 29.85% of the mucoadhesiveness of the film containing tannin, as compared to the reference, prolongs the bioavailability of the active substance; a fact also demonstrated by the controlled release studies. The presence of bioactive principles, as well as tannins and lipoic acid, gives biomaterials an antioxidant capacity on average 40%–50% higher compared to the base matrix. The results of the tests of the mechanical resistance, mucoadhesiveness, bioadhesiveness, water absorption and antioxidant capacity of active principles recommend these biomaterials for the manufacture of cosmetic masks or patches. Full article

(This article belongs to the Special Issue Functional Chitosan-Based Composites)

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17 pages, 4758 KiB

Open AccessArticle

Chitosan-Sulfated Titania Composite Membranes with Potential Applications in Fuel Cell: Influence of Cross-Linker Nature

by Andra-Cristina Humelnicu, Petrisor Samoila, Mihai Asandulesa, Corneliu Cojocaru, Adrian Bele, Adriana T. Marinoiu, Ada Sacca and Valeria Harabagiu

Polymers 2020, 12(5), 1125; https://doi.org/10.3390/polym12051125 - 14 May 2020

Cited by 19 | Viewed by 2346

Abstract

Chitosan-sulfated titania composite membranes were prepared, characterized, and evaluated for potential application as polymer electrolyte membranes. To improve the chemical stability, the membranes were cross-linked using sulfuric acid, pentasodium triphosphate, and epoxy-terminated polydimethylsiloxane. Differences in membranes’ structure, thickness, morphology, mechanical, and thermal properties prior and after cross-linking reactions were evaluated. Membranes’ water uptake capacities and their chemical stability in Fenton reagent were also studied. As proved by dielectric spectroscopy, the conductivity strongly depends on cross-linker nature and on hydration state of membranes. The most encouraging results were obtained for the chitosan-sulfated titania membrane cross-linked with sulfuric acid. This hydrated membrane attained values of proton conductivity of 1.1 × 10⁻³ S/cm and 6.2 × 10⁻³ S/cm, as determined at 60 °C by dielectric spectroscopy and the four-probes method, respectively. Full article

(This article belongs to the Special Issue Functional Chitosan-Based Composites)

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13 pages, 3444 KiB

Open AccessArticle

Dynamics and Rheological Behavior of Chitosan-Grafted-Polyacrylamide in Aqueous Solution upon Heating

by Mengjie Wang, Yonggang Shangguan and Qiang Zheng

Polymers 2020, 12(4), 916; https://doi.org/10.3390/polym12040916 - 15 Apr 2020

Cited by 5 | Viewed by 2280

Abstract

In this work, the transformation of chitosan-grafted-polyacrylamide (GPAM) aggregates in aqueous solution upon heating was explored by cryo-electron microscope (cryo-TEM) and dynamic light scattering (DLS), and larger aggregates were formed in GPAM aqueous solution upon heating, which were responsible for the thermo-thickening behavior of GPAM aqueous solution during the heating process. The heating initiates a transformation from H-bonding aggregates to a large-sized cluster formed by self-assembled hydrophobic chitosan backbones. The acetic acid (HAc) concentration has a significant effect on the thermo-thickening behavior of GPAM aqueous solution; there is a critical value of the concentration (>0.005 M) for the thermo-thickening of 10 mg/mL GPAM solution. The concentration of HAc will affect the protonation degree of GPAM, and affect the strength of the electrostatic repulsion between GPAM molecular segments, which will have a significant effect on the state of the aggregates in solution. Other factors that have an influence on the thermo-thickening behavior of GPAM aqueous solution upon heating were investigated and discussed in detail, including the heating rate and shear rate. Full article

(This article belongs to the Special Issue Functional Chitosan-Based Composites)

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Review

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24 pages, 3183 KiB

Open AccessEditor’s ChoiceReview

Chitosan-Based Drug Delivery System: Applications in Fish Biotechnology

by Yuanbing Wu, Ania Rashidpour, María Pilar Almajano and Isidoro Metón

Polymers 2020, 12(5), 1177; https://doi.org/10.3390/polym12051177 - 21 May 2020

Cited by 65 | Viewed by 7279

Abstract

Chitosan is increasingly used for safe nucleic acid delivery in gene therapy studies, due to well-known properties such as bioadhesion, low toxicity, biodegradability and biocompatibility. Furthermore, chitosan derivatization can be easily performed to improve the solubility and stability of chitosan–nucleic acid polyplexes, and enhance efficient target cell drug delivery, cell uptake, intracellular endosomal escape, unpacking and nuclear import of expression plasmids. As in other fields, chitosan is a promising drug delivery vector with great potential for the fish farming industry. This review highlights state-of-the-art assays using chitosan-based methodologies for delivering nucleic acids into cells, and focuses attention on recent advances in chitosan-mediated gene delivery for fish biotechnology applications. The efficiency of chitosan for gene therapy studies in fish biotechnology is discussed in fields such as fish vaccination against bacterial and viral infection, control of gonadal development and gene overexpression and silencing for overcoming metabolic limitations, such as dependence on protein-rich diets and the low glucose tolerance of farmed fish. Finally, challenges and perspectives on the future developments of chitosan-based gene delivery in fish are also discussed. Full article

(This article belongs to the Special Issue Functional Chitosan-Based Composites)

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