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Special Issue "Bridging Polysaccharides from Nature to Products: Fundamentals and Technology"

A special issue of International Journal of Molecular Sciences (ISSN 1422-0067). This special issue belongs to the section "Macromolecules".

Deadline for manuscript submissions: closed (18 December 2020).

Special Issue Editors

Prof. Dr. Artur J.M. Valente
E-Mail Website
Guest Editor
Centro de Química, Department of Chemistry, University of Coimbra, 3004-535 Coimbra, Portugal
Interests: hydrogels and biogels; polyelectrolytes; water soluble conjugated polymers; transport properties; interface phenomena; oligosaccharides
Special Issues, Collections and Topics in MDPI journals
Prof. Dr. Edvani C. Muniz
E-Mail Website
Guest Editor
1. Department of Chemistry, State University of Maringá, UEM, Maringá 87020-900, Brazil
2. Department of Chemistry, Federal University of Piauí, Teresina CEP 64049-550, Brazil
Interests: chemical and physical hydrogels; chemical modification of polysaccharides; drug delivery from polymeric matrix; chemical recycling of polymers; electrospinning of polymers
Special Issues, Collections and Topics in MDPI journals
Prof. Dr. Pietro Matricardi
E-Mail Website
Guest Editor
Department of Drug Chemistry and Technologies, Faculty of Pharmacy and Medicine, "Sapienza" University of Rome, Rome, Italy
Interests: polysaccharide; hydrogels; nanohydrogels; drug delivery; tissue engineering
Special Issues, Collections and Topics in MDPI journals
Prof. Dr. You-Lo Hsieh
E-Mail Website
Guest Editor
Department of Biological and Agricultural Engineering, University of California, Davis, CA 95616, USA
Interests: biopolymer functional materials; nanocelluloses; micro-, meso-, and macro-porous materials; hierarchical hybrids and fibers

Special Issue Information

Dear Colleagues,

Polysaccharides are among the most abundant polymers in nature; they are found in plants and marine and terrestrial organisms. Common polysaccharides include cellulose, chitin, chitosan, starch, pectin, hyaluronic acid, alginate, carrageenan, and chondroitin sulfate. Polysaccharides have general biocompatibility (nontoxicity) and biodegradability, which is why these macromolecules are widely used in pharmaceutical, biomedical, and biotechnological applications. They also form easily 3D cross-linked structures, allowing their applications in pharmaceutical and environmental sciences. They are also extensively used as gelling agents, thickeners, stabilizers, and emulsifiers in food products. The presence of functional groups along the polymer chains allows their easy chemical functionalization, thus extending the exploitation opportunities.

This Special Issue aims to highlight fundamental and applied aspects of advanced research on polysaccharides in different fields including, but not limited to, biomedical, biochemistry, food chemistry, drug delivery, environmental science, and biorefinery and paper industry.

Prof. Dr. Pietro Matricardi
Prof. Dr. You-Lo Hsieh
Prof. Dr. Artur J.M. Valente
Prof. Dr. Edvani C. Muniz
Guest Editors

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

  • biomedical applications
  • biocompatibility and biological functions
  • cellulose dissolution
  • drug delivery
  • food chemistry
  • functional materials
  • hydrogels
  • nanoparticles and nanofibers
  • polysaccharides
  • tissue engineering

Related Special Issue

Published Papers (10 papers)

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Research

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Article
The Simple Method of Preparation of Highly Carboxylated Bacterial Cellulose with Ni- and Mg-Ferrite-Based Versatile Magnetic Carrier for Enzyme Immobilization
Int. J. Mol. Sci. 2021, 22(16), 8563; https://0-doi-org.brum.beds.ac.uk/10.3390/ijms22168563 - 09 Aug 2021
Cited by 1 | Viewed by 692
Abstract
The bacterial cellulose (BC) is a versatile biopolymer of microbial origin characterized by high purity and unusual water and material properties. However, the native BC contains a low number of functional groups, which significantly limits its further application. The main goal of its [...] Read more.
The bacterial cellulose (BC) is a versatile biopolymer of microbial origin characterized by high purity and unusual water and material properties. However, the native BC contains a low number of functional groups, which significantly limits its further application. The main goal of its effective modification is to use methods that allow the unusual properties of BC to be retained and the desired functional group to be efficiently introduced. In the present study, the new magnetic carrier based on functionalized citric acid (CA) bacterial cellulose was developed and tested to support critical industrial enzymes such as lipase B from Candida antarctica and phospholipase A from Aspergillus oryzae. The applied method allowed BC to be effectively modified by citric acid and a sufficient number of carboxylic groups to be introduced, up to 3.6 mmol of COOH per gram of dry mass of the prepared carrier. The DSC and TGA analyses revealed carrier stability at operational temperatures in the range of 20 °C to 100 °C and substantially influenced the amount of the introduced carboxyl groups on carrier properties. Both enzymes’ immobilization significantly improves their thermal stability at 60 °C without a significant thermal and pH optima effect. The analyzed enzymes showed good operational stability with a significant residual activity after ten cycles of repeated uses. The new magnetic carrier based on highly carboxylated bacterial cellulose has a high application capability as matrix for immobilization the various enzymes of industrial interest. Full article
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Article
Hybrid Methacrylated Gelatin and Hyaluronic Acid Hydrogel Scaffolds. Preparation and Systematic Characterization for Prospective Tissue Engineering Applications
Int. J. Mol. Sci. 2021, 22(13), 6758; https://0-doi-org.brum.beds.ac.uk/10.3390/ijms22136758 - 23 Jun 2021
Cited by 3 | Viewed by 838
Abstract
Hyaluronic acid (HA) and gelatin (Gel) are major components of the extracellular matrix of different tissues, and thus are largely appealing for the construction of hybrid hydrogels to combine the favorable characteristics of each biopolymer, such as the gel adhesiveness of Gel and [...] Read more.
Hyaluronic acid (HA) and gelatin (Gel) are major components of the extracellular matrix of different tissues, and thus are largely appealing for the construction of hybrid hydrogels to combine the favorable characteristics of each biopolymer, such as the gel adhesiveness of Gel and the better mechanical strength of HA, respectively. However, despite previous studies conducted so far, the relationship between composition and scaffold structure and physico-chemical properties has not been completely and systematically established. In this work, pure and hybrid hydrogels of methacroyl-modified HA (HAMA) and Gel (GelMA) were prepared by UV photopolymerization and an extensive characterization was done to elucidate such correlations. Methacrylation degrees of ca. 40% and 11% for GelMA and HAMA, respectively, were obtained, which allows to improve the hydrogels’ mechanical properties. Hybrid GelMA/HAMA hydrogels were stiffer, with elastic modulus up to ca. 30 kPa, and porous (up to 91%) compared with pure GelMA ones at similar GelMA concentrations thanks to the interaction between HAMA and GelMA chains in the polymeric matrix. The progressive presence of HAMA gave rise to scaffolds with more disorganized, stiffer, and less porous structures owing to the net increase of mass in the hydrogel compositions. HAMA also made hybrid hydrogels more swellable and resistant to collagenase biodegradation. Hence, the suitable choice of polymeric composition allows to regulate the hydrogels´ physical properties to look for the most optimal characteristics required for the intended tissue engineering application. Full article
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Article
Effect of Hofmeister Ions on Transport Properties of Aqueous Solutions of Sodium Hyaluronate
Int. J. Mol. Sci. 2021, 22(4), 1932; https://0-doi-org.brum.beds.ac.uk/10.3390/ijms22041932 - 16 Feb 2021
Cited by 1 | Viewed by 642
Abstract
Tracer diffusion coefficients obtained from the Taylor dispersion technique at 25.0 °C were measured to study the influence of sodium, ammonium and magnesium salts at 0.01 and 0.1 mol dm−3 on the transport behavior of sodium hyaluronate (NaHy, 0.1%). The selection of [...] Read more.
Tracer diffusion coefficients obtained from the Taylor dispersion technique at 25.0 °C were measured to study the influence of sodium, ammonium and magnesium salts at 0.01 and 0.1 mol dm−3 on the transport behavior of sodium hyaluronate (NaHy, 0.1%). The selection of these salts was based on their position in Hofmeister series, which describe the specific influence of different ions (cations and anions) on some physicochemical properties of a system that can be interpreted as a salting-in or salting-out effect. In our case, in general, an increase in the ionic strength (i.e., concentrations at 0.01 mol dm−3) led to a significant decrease in the limiting diffusion coefficient of the NaHy 0.1%, indicating, in those circumstances, the presence of salting-in effects. However, the opposite effect (salting-out) was verified with the increase in concentration of some salts, mainly for NH4SCN at 0.1 mol dm−3. In this particular salt, the cation is weakly hydrated and, consequently, its presence does not favor interactions between NaHy and water molecules, promoting, in those circumstances, less resistance to the movement of NaHy and thus to the increase of its diffusion (19%). These data, complemented by viscosity measurements, permit us to have a better understanding about the effect of these salts on the transport behaviour of NaHy. Full article
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Article
Effect of O-Antigen Chain Length Regulation on the Immunogenicity of Shigella and Salmonella Generalized Modules for Membrane Antigens (GMMA)
Int. J. Mol. Sci. 2021, 22(3), 1309; https://0-doi-org.brum.beds.ac.uk/10.3390/ijms22031309 - 28 Jan 2021
Cited by 4 | Viewed by 789
Abstract
Recently, generalized modules for membrane antigens (GMMA) technology has been proposed as an alternative approach to traditional glycoconjugate vaccines for O-antigen delivery. Saccharide length is a well-known parameter that can impact the immune response induced by glycoconjugates both in terms of magnitude and [...] Read more.
Recently, generalized modules for membrane antigens (GMMA) technology has been proposed as an alternative approach to traditional glycoconjugate vaccines for O-antigen delivery. Saccharide length is a well-known parameter that can impact the immune response induced by glycoconjugates both in terms of magnitude and quality. However, the criticality of O-antigen length on the immune response induced by GMMA-based vaccines has not been fully elucidated. Here, Shigella and Salmonella GMMA-producing strains were further mutated in order to display homogeneous polysaccharide populations of different sizes on a GMMA surface. Resulting GMMA were compared in mice immunization studies. Athymic nude mice were also used to investigate the involvement of T-cells in the immune response elicited. In contrast with what has been reported for traditional glycoconjugate vaccines and independent of the pathogen and the sugar structural characteristics, O-antigen length did not result in being a critical parameter for GMMA immunogenicity. This work supports the identification of critical quality attributes to optimize GMMA vaccine design and improve vaccine efficacy and gives insights on the nature of the immune response induced by GMMA. Full article
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Article
Polymer-Decorated Cellulose Nanocrystals as Environmentally Friendly Additives for Olefin-Based Drilling Fluids
Int. J. Mol. Sci. 2021, 22(1), 352; https://0-doi-org.brum.beds.ac.uk/10.3390/ijms22010352 - 31 Dec 2020
Cited by 3 | Viewed by 859
Abstract
In this study, we intended to evaluate the performance of olefin-based drilling fluids after addition of cellulose nanocrystal (CNC) derivatives. For this purpose, firstly, cellulose nanocrystals, produced from sulfuric acid hydrolysis of cotton fibers, were functionalized with poly(N-isopropylacrylamide) (PNIPAM) chains via [...] Read more.
In this study, we intended to evaluate the performance of olefin-based drilling fluids after addition of cellulose nanocrystal (CNC) derivatives. For this purpose, firstly, cellulose nanocrystals, produced from sulfuric acid hydrolysis of cotton fibers, were functionalized with poly(N-isopropylacrylamide) (PNIPAM) chains via free radicals. The samples were then characterized via Fourier transform infrared spectroscopy (FTIR), nuclear magnetic resonance (NMR), X-ray diffraction (XRD), thermogravimetric analysis (TGA), confocal microscopy, dynamic light scattering (DLS), and zeta potential measurements in water. The FTIR and NMR spectra exhibited the characteristic signals of CNC and PNIPAM groups, indicating successful grafting. As expected, X-ray diffractograms showed that the crystallinity of CNCs reduces after chemical modification. TGA revealed that the surface-functionalized CNCs present higher thermal stability than pure CNCs. The confocal microscopy, zeta potential, and DLS results were consistent with the behavior of cellulose nanocrystals decorated by a shell of PNIPAM chains. The fluids with a small amount of modified CNCs presented a much lower volume of filtrate after high-temperature and high-pressure (HTHP) filtration tests than the corresponding standard fluid, indicating the applicability of the environmentally friendly particles for olefin-based drilling fluids. Full article
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Article
Tedizolid-Cyclodextrin System as Delayed-Release Drug Delivery with Antibacterial Activity
Int. J. Mol. Sci. 2021, 22(1), 115; https://0-doi-org.brum.beds.ac.uk/10.3390/ijms22010115 - 24 Dec 2020
Cited by 4 | Viewed by 798
Abstract
Progressive increase in bacterial resistance has caused an urgent need to introduce new antibiotics, one of them being oxazolidinones with their representative tedizolid. Despite the broad spectrum of activity of the parent tedizolid, it is characterized by low water solubility, which limits its [...] Read more.
Progressive increase in bacterial resistance has caused an urgent need to introduce new antibiotics, one of them being oxazolidinones with their representative tedizolid. Despite the broad spectrum of activity of the parent tedizolid, it is characterized by low water solubility, which limits its use. The combination of the active molecule with a multifunctional excipient, which is cyclodextrins, allows preservation of its pharmacological activity and modification of its physicochemical properties. Therefore, the aim of the study was to change the dissolution rate and permeability through the model membrane of tedizolid by formation of solid dispersions with a cyclodextrin. The research included identification of tedizolid-hydroxypropyl-β-cyclodextrin (tedizolid/HP-β-CD) inclusion complex by thermal method (Differential Scanning Colorimetry), spectroscopic methods (powder X-ray diffraction, Fourier-Transform Infrared spectroscopy), and molecular docking. The second part of the research concerned the physicochemical properties (dissolution and permeability) and the biological properties of the system in terms of its microbiological activity. An increase in the dissolution rate was observed in the presence of cyclodextrin, while maintaining a high permeation coefficient and high microbiological activity. The proposed approach is an opportunity to develop drug delivery systems used in the treatment of resistant bacterial infections, in which, in addition to modifying the physicochemical properties caused by cyclodextrin, we observe a favorable change in the pharmacological potential of the bioactives. Full article
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Article
Bactericidal Pectin/Chitosan/Glycerol Films for Food Pack Coatings: A Critical Viewpoint
Int. J. Mol. Sci. 2020, 21(22), 8663; https://0-doi-org.brum.beds.ac.uk/10.3390/ijms21228663 - 17 Nov 2020
Cited by 6 | Viewed by 1035
Abstract
Pectin and chitosan films containing glycerol (Gly) at 5, 10, 15, 20, 30, and 40 wt % were prepared in an aqueous HCl solution (0.10 M) by the solvent evaporation method. The unwashed film (UF) containing 40 wt % Gly (UF40) had elongation [...] Read more.
Pectin and chitosan films containing glycerol (Gly) at 5, 10, 15, 20, 30, and 40 wt % were prepared in an aqueous HCl solution (0.10 M) by the solvent evaporation method. The unwashed film (UF) containing 40 wt % Gly (UF40) had elongation at break (ε, %) of 19%. Washed films (WFs) had high tensile strength (σ > 46 MPa) and low elongation at break (ε, <5.0%), enabling their use in food packaging applications. The polymers’ self-assembling occurred during the washing, increasing the stiffness. The XPS analysis suggests that some HCl is lost during the drying process, resulting in a low acid content on the UF surfaces. The UF40 (at 5.0 mg/mL) exhibits cytocompatibility toward mammalian cells and antimicrobial and anti-adhesive properties against Escherichia coli. The remaining HCl in the UF40 can be a disadvantage for food packaging applications; the UF40 (∅ = 8.5 mm; 55 μm thickness) releases H3O+/HCl, reducing the pH to approximately 3.0 when kept in 200 mL distilled water for approximately 30 min. Therefore, we propose the use of UF40 to coat commercial food packaging. The UF40 has low permeability to water vapor and oxygen and works as a barrier against ultraviolet light. The UF40 is also colorless and completely transparent. The UF40 maintained tomatoes’ structural integrity for 18 days at room temperature with no oxidation or microorganism contamination. This paper presents a critical viewpoint concerning chitosan-based films with antimicrobial activities. Full article
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Article
On the Mechanism of Genipin Binding to Primary Amines in Lactose-Modified Chitosan at Neutral pH
Int. J. Mol. Sci. 2020, 21(18), 6831; https://0-doi-org.brum.beds.ac.uk/10.3390/ijms21186831 - 17 Sep 2020
Cited by 3 | Viewed by 763
Abstract
The present manuscript deals with the elucidation of the mechanism of genipin binding by primary amines at neutral pH. UV-VIS and CD measurements both in the presence of oxygen and in oxygen-depleted conditions, combined with computational analyses, led to propose a novel mechanism [...] Read more.
The present manuscript deals with the elucidation of the mechanism of genipin binding by primary amines at neutral pH. UV-VIS and CD measurements both in the presence of oxygen and in oxygen-depleted conditions, combined with computational analyses, led to propose a novel mechanism for the formation of genipin derivatives. The indications collected with chiral and achiral primary amines allowed interpreting the genipin binding to a lactose-modified chitosan (CTL or Chitlac), which is soluble at all pH values. Two types of reaction and their kinetics were found in the presence of oxygen: (i) an interchain reticulation, which involves two genipin molecules and two polysaccharide chains, and (ii) a binding of one genipin molecule to the polymer chain without chain–chain reticulation. The latter evolves in additional interchain cross-links, leading to the formation of the well-known blue iridoid-derivatives. Full article
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Article
Chitosan-Based Coacervate Polymers for Propolis Encapsulation: Release and Cytotoxicity Studies
Int. J. Mol. Sci. 2020, 21(12), 4561; https://0-doi-org.brum.beds.ac.uk/10.3390/ijms21124561 - 26 Jun 2020
Cited by 11 | Viewed by 1352
Abstract
Chitosan-DNA (CS-DNA) and Chitosan-Pectin (CS-P) hydrogels were formulated as a sustained drug delivery carrier for drug delivery. For this, hydrogels were prepared by emulsion technique: mixing aqueous phase of the CS and DNA or P solution with benzyl alcohol using a high-performance dispersing [...] Read more.
Chitosan-DNA (CS-DNA) and Chitosan-Pectin (CS-P) hydrogels were formulated as a sustained drug delivery carrier for drug delivery. For this, hydrogels were prepared by emulsion technique: mixing aqueous phase of the CS and DNA or P solution with benzyl alcohol using a high-performance dispersing instrument. Green Propolis (GP) was incorporated by imbibition: hydrogels were placed in GP aqueous solution (70 µg/mL) for 2 h. The specimens were freeze-dried and then characterized using different techniques. In vitro cell viability and morphology were also performed using the MG63 cell line. The presence of P was evidenced by the occurrence of a strong band at 1745 cm−1, also occurring in the blend. DNA and CS-DNA showed a strong band at 1650 cm−1, slightly shifted from the chitosan band. The sorption of GP induced a significant modification of the gel surface morphology and some phase separation occurs between chitosan and DNA. Drug release kinetics in water and in saliva follow a two-step mechanism. Significant biocompatibility revealed that these hydrogels were non-toxic and provided acceptable support for cell survival. Thus, the hydrogel complexation of chitosan with DNA and with Pectin provides favorable micro-environment for cell growth and is a viable alternative drug delivery system for Green Propolis. Full article
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Review

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Review
Versatile Types of Polysaccharide-Based Drug Delivery Systems: From Strategic Design to Cancer Therapy
Int. J. Mol. Sci. 2020, 21(23), 9159; https://0-doi-org.brum.beds.ac.uk/10.3390/ijms21239159 - 01 Dec 2020
Cited by 10 | Viewed by 954
Abstract
Chemotherapy is still the most direct and effective means of cancer therapy nowadays. The proposal of drug delivery systems (DDSs) has effectively improved many shortcomings of traditional chemotherapy drugs. The technical support of DDSs lies in their excellent material properties. Polysaccharides include a [...] Read more.
Chemotherapy is still the most direct and effective means of cancer therapy nowadays. The proposal of drug delivery systems (DDSs) has effectively improved many shortcomings of traditional chemotherapy drugs. The technical support of DDSs lies in their excellent material properties. Polysaccharides include a series of natural polymers, such as chitosan, hyaluronic acid, and alginic acid. These polysaccharides have good biocompatibility and degradability, and they are easily chemical modified. Therefore, polysaccharides are ideal candidate materials to construct DDSs, and their clinical application prospects have been favored by researchers. On the basis of versatile types of polysaccharides, this review elaborates their applications from strategic design to cancer therapy. The construction and modification methods of polysaccharide-based DDSs are specifically explained, and the latest research progress of polysaccharide-based DDSs in cancer therapy are also summarized. The purpose of this review is to provide a reference for the design and preparation of polysaccharide-based DDSs with excellent performance. Full article
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