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Polymers
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Functional Gelatin
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Functional Gelatin

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 (31 October 2020) | Viewed by 41801

Special Issue Editor

Prof. Dr. Svetlana Deckach

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Guest Editor
Chemistry Department, Murmansk State Technical University, Murmansk, Russia
Interests: macromolecules; biopolymers; proteins; drug-delivery systems; colloid and surface chemistry; rheology; pharmaceutical chemistry
Special Issues, Collections and Topics in MDPI journals

Special Issue Information

Dear Colleagues,

Gelatin—the product of the breakdown of the fibrillar protein collagen—is one of the most widely used natural biopolymers in the industry. The surface activity and the unique ability of the thermo-reversible structure formation determine the demand for gelatin in various fields, including the food industry, medicine, pharmaceuticals, biotechnology, and so on. Gelatin exhibits its properties most clearly in multicomponent systems. A deliberate change in the properties of gelatin, resulting from its complexation with surfactants, polysaccharides, polyelectrolytes, and so on, is the key for industrial use, and, above all, for food technologies. The relationship between molecular weight distribution, secondary structure and functional properties, structural stability and rheological behavior, interactions between complexing components, distribution between the bulk phases and various kinds of interfaces, are basic aspects of this field. This Special Issue welcomes all contributions from a comprehensive range of expertise in the field. Subjects like phase separation, surface phenomena, drug delivery, foams, emulsions, gels, and 3D printing are welcome. Proposals are also welcome from the many industries that manufacture gelatins or gelatin products, including food, pharmaceutical, cosmetic, and medicine industries, to name a few.

Prof. Svetlana Derkatch
Guest Editor

Manuscript Submission Information

Manuscripts should be submitted online at www.mdpi.com by registering and logging in to this website. Once you are registered, click here to go to the submission form. Manuscripts can be submitted until the deadline. All submissions that pass pre-check are peer-reviewed. Accepted papers will be published continuously in the journal (as soon as accepted) and will be listed together on the special issue website. Research articles, review articles as well as short communications are invited. For planned papers, a title and short abstract (about 100 words) can be sent to the Editorial Office for announcement on this website.

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. Polymers 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 2700 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.

Published Papers (10 papers)

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Research

17 pages, 5166 KiB  
Article
Rheological Properties of Fish Gelatin Modified with Sodium Alginate
by Svetlana R. Derkach, Daria S. Kolotova, Nikolay G. Voron’ko, Ekaterina D. Obluchinskaya and Alexander Ya. Malkin
Polymers 2021, 13(5), 743; https://0-doi-org.brum.beds.ac.uk/10.3390/polym13050743 - 27 Feb 2021
Cited by 23 | Viewed by 3053
Abstract
Polyelectrolyte complexes of sodium alginate and gelatin obtained from cold-blooded fish were studied for potential application as structure-forming agents in food hydrogels. The mass ratio of sodium alginate to gelatin plays a decisive role in the sol-gel transition and rheological behavior of the [...] Read more.
Polyelectrolyte complexes of sodium alginate and gelatin obtained from cold-blooded fish were studied for potential application as structure-forming agents in food hydrogels. The mass ratio of sodium alginate to gelatin plays a decisive role in the sol-gel transition and rheological behavior of the complexes. Differences in the sol-gel transition temperature were observed upon heating and cooling, as is typical for such materials. We investigated the characteristics of this transition by measuring the isothermal changes in the elastic modulus over time at a constant frequency and the transition temperature at a range of frequencies. The kinetic nature of this transition depends on the composition of the complexes. A characteristic alginate-gelatin mass ratio is the ratio at which maximum transition temperature as well as elastic modulus and viscosity (rheological parameters) values are obtained; the characteristic mass ratio for these complexes was found to be 0.06. Calculation of the ionic group ratios in the biopolymers that form complexes and comparison of these data with the turbidimetric titration results clarified the origin of these maxima. Measuring the viscoelastic properties and the creep-elastic recoil of the samples allowed us to characterize these materials as viscoelastic media with a viscosity in the order of 103–104 Pa·s and an elastic modulus in the order of 102–103 Pa. These values drastically decrease at a certain stress threshold, which can be treated as the gel strength limit. Therefore, the observed rheological behavior of gels formed by fish gelatin modified with sodium alginate characterizes them as typical viscoelastic soft matter. Full article
(This article belongs to the Special Issue Functional Gelatin)
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15 pages, 2719 KiB  
Article
Chronic High Glucose Concentration Induces Inflammatory and Remodeling Changes in Valvular Endothelial Cells and Valvular Interstitial Cells in a Gelatin Methacrylate 3D Model of the Human Aortic Valve
by Letitia Ciortan, Razvan Daniel Macarie, Sergiu Cecoltan, Mihaela Vadana, Monica Madalina Tucureanu, Andreea Cristina Mihaila, Ionel Droc, Elena Butoi and Ileana Manduteanu
Polymers 2020, 12(12), 2786; https://0-doi-org.brum.beds.ac.uk/10.3390/polym12122786 - 25 Nov 2020
Cited by 21 | Viewed by 2889
Abstract
Calcific aortic valve disease (CAVD), a degenerative disease characterized by inflammation, fibrosis and calcification, is accelerated in diabetes. Hyperglycemia contributes to this process by mechanisms that still need to be uncovered. We have recently developed a 3D model of the human aortic valve [...] Read more.
Calcific aortic valve disease (CAVD), a degenerative disease characterized by inflammation, fibrosis and calcification, is accelerated in diabetes. Hyperglycemia contributes to this process by mechanisms that still need to be uncovered. We have recently developed a 3D model of the human aortic valve based on gelatin methacrylate and revealed that high glucose (HG) induced osteogenic molecules and increased calcium deposits in a pro-osteogenic environment. To further understand the events leading to calcification in diabetic conditions in CAVD, we analyzed here the inflammatory and remodeling mechanisms induced by HG in our 3D model. We exposed valvular endothelial cells (VEC) and interstitial cells (VIC) to normal glucose (NG) or HG for 7 and 14 days, then we isolated and separated the cells by anti-CD31 immunomagnetic beads. The changes induced by HG in the 3D model were investigated by real-time polymerase chain reaction (RT-PCR), Western blot, enzyme-linked immunosorbent assay (ELISA) and immunofluorescence. Our results showed that HG induced expression of different cytokines, cell adhesion molecules and matrix metalloproteinases in VEC and VIC. In addition, protein kinase C was increased in VEC and VIC, indicating molecular mechanisms associated with HG induced inflammation and remodeling in both valvular cells. These findings may indicate new biomarkers and targets for therapy in diabetes associated with CAVD. Full article
(This article belongs to the Special Issue Functional Gelatin)
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16 pages, 8733 KiB  
Article
Enzyme-Crosslinked Electrospun Fibrous Gelatin Hydrogel for Potential Soft Tissue Engineering
by Kexin Nie, Shanshan Han, Jianmin Yang, Qingqing Sun, Xiaofeng Wang, Xiaomeng Li and Qian Li
Polymers 2020, 12(9), 1977; https://0-doi-org.brum.beds.ac.uk/10.3390/polym12091977 - 31 Aug 2020
Cited by 32 | Viewed by 4184
Abstract
Soft tissue engineering has been seeking ways to mimic the natural extracellular microenvironment that allows cells to migrate and proliferate to regenerate new tissue. Therefore, the reconstruction of soft tissue requires a scaffold possessing the extracellular matrix (ECM)-mimicking fibrous structure and elastic property, [...] Read more.
Soft tissue engineering has been seeking ways to mimic the natural extracellular microenvironment that allows cells to migrate and proliferate to regenerate new tissue. Therefore, the reconstruction of soft tissue requires a scaffold possessing the extracellular matrix (ECM)-mimicking fibrous structure and elastic property, which affect the cell functions and tissue regeneration. Herein, an effective method for fabricating nanofibrous hydrogel for soft tissue engineering is demonstrated using gelatin–hydroxyphenylpropionic acid (Gel–HPA) by electrospinning and enzymatic crosslinking. Gel–HPA fibrous hydrogel was prepared by crosslinking the electrospun fibers in ethanol-water solution with an optimized concentration of horseradish peroxidase (HRP) and H2O2. The prepared fibrous hydrogel held the soft and elastic mechanical property of hydrogels and the three-dimensional (3D) fibrous structure of electrospun fibers. It was proven that the hydrogel scaffolds were biocompatible, improving the cellular adhesion, spreading, and proliferation. Moreover, the fibrous hydrogel showed rapid biodegradability and promoted angiogenesis in vivo. Overall, this study represents a novel biomimetic approach to generate Gel–HPA fibrous hydrogel scaffolds which have excellent potential in soft tissue regeneration applications. Full article
(This article belongs to the Special Issue Functional Gelatin)
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15 pages, 5024 KiB  
Article
Bioinspired Hydrogel Coating Based on Methacryloyl Gelatin Bioactivates Polypropylene Meshes for Abdominal Wall Repair
by Andrada Serafim, Sergiu Cecoltan, Elena Olăreț, Diana-Maria Dragusin, Eugeniu Vasile, Valentin Popescu, Bogdan Stelian Manolescu Mastalier, Horia Iovu and Izabela-Cristina Stancu
Polymers 2020, 12(8), 1677; https://0-doi-org.brum.beds.ac.uk/10.3390/polym12081677 - 28 Jul 2020
Cited by 16 | Viewed by 3404
Abstract
Considering the potential of hydrogels to mimic the cellular microenvironment, methacryloyl gelatin (GelMA) and methacryloyl mucin (MuMA) were selected and compared as bioinspired coatings for commercially available polypropylene (PP) meshes for ventral hernia repair. Thin, elastic hydrated hydrogel layers were obtained through network-forming [...] Read more.
Considering the potential of hydrogels to mimic the cellular microenvironment, methacryloyl gelatin (GelMA) and methacryloyl mucin (MuMA) were selected and compared as bioinspired coatings for commercially available polypropylene (PP) meshes for ventral hernia repair. Thin, elastic hydrated hydrogel layers were obtained through network-forming photo-polymerization, after immobilization of derivatives on the surface of the PP fibers. Fourier transform infrared spectroscopy (FTIR) proved the successful coating while the surface morphology and homogeneity were investigated by scanning electron microscopy (SEM) and micro-computed tomography (micro-CT). The stability of the hydrogel layers was evaluated through biodynamic tests performed on the coated meshes for seven days, followed by inspection of surface morphology through SEM and micro-CT. Taking into account that platelet-rich plasma (PRP) may improve healing due to its high concentration of growth factors, this extract was used as pre-treatment for the hydrogel coating to additionally stimulate cell interactions. The performed advanced characterization proved that GelMA and MuMA coatings can modulate fibroblasts response on PP meshes, either as such or supplemented with PRP extract as a blood-derived bioactivator. GelMA supported the best cellular response. These findings may extend the applicative potential of functionalized gelatin opening a new path on the research and engineering of a new generation of bioactive meshes. Full article
(This article belongs to the Special Issue Functional Gelatin)
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23 pages, 3218 KiB  
Article
Characterization and Application of Gelatin Films with Pecan Walnut and Shell Extract (Carya illinoiensis)
by Juliana Villasante, Anna Martin-Lujano and María Pilar Almajano
Polymers 2020, 12(6), 1424; https://0-doi-org.brum.beds.ac.uk/10.3390/polym12061424 - 26 Jun 2020
Cited by 19 | Viewed by 3222
Abstract
Phenolic compounds that come from natural products are a good option for minimizing lipid oxidation. It should be noted that these are not only introduced directly into the food, but also incorporated into edible biofilms. In contact with food, they extend its useful [...] Read more.
Phenolic compounds that come from natural products are a good option for minimizing lipid oxidation. It should be noted that these are not only introduced directly into the food, but also incorporated into edible biofilms. In contact with food, they extend its useful life by avoiding contact with other surface and preventing deterioration air, one of the main objectives. In particular, gelatin is a biopolymer that has a great potential due to its abundance, low cost and good film-forming capacity. The aim of this study has been to design and analyse gelatin films that incorporate bioactive compounds that come from the walnut and a by-product, the walnut shell. The results showed that mechanical and water vapor barrier properties of the developed films varied depending on the concentration of the walnut, shell and synthetic antioxidant. With increasing walnut concentration (15%) the permeability to water vapor (0.414 g·mm/m2·day·Pascal, g·mm/m2·day·Pa) was significantly lower than the control (5.0368 g·mm/m2·day·Pa). Furthermore, in the new films the elongation at the break and Young’s modulus decrease by six times with respect to the control. Films with pure gelatin cannot act as an antioxidant shield to prevent food oxidation, but adding pecan walnut (15% concentration) presents 30% inhibition of the DPPH stable radical. Furthermore, in the DSC, the addition of walnut (15 and 9% concentrations), showed the formation of big crystals; which could improve the thermal stability of gelatin films. The use of new gelatin films has shown good protection against the oxidation of beef patties, increasing the useful lifetime up to nine days, compared to the control (3–4 days), which opens up a big field to the commercialization of meat products with lower quantities of synthetic products. Full article
(This article belongs to the Special Issue Functional Gelatin)
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14 pages, 1781 KiB  
Article
Fabrication and Characterization of Hydrogels Based on Gelatinised Collagen with Potential Application in Tissue Engineering
by Victor Perez-Puyana, Mercedes Jiménez-Rosado, Alberto Romero and Antonio Guerrero
Polymers 2020, 12(5), 1146; https://0-doi-org.brum.beds.ac.uk/10.3390/polym12051146 - 17 May 2020
Cited by 19 | Viewed by 4188
Abstract
Regenerative medicine is increasingly focused on the development of biomaterials that facilitate cell adhesion and proliferation through the use of natural polymers, which have better biocompatibility and biodegradability. In this way, the use of hydrogels has been considered as a potential option for [...] Read more.
Regenerative medicine is increasingly focused on the development of biomaterials that facilitate cell adhesion and proliferation through the use of natural polymers, which have better biocompatibility and biodegradability. In this way, the use of hydrogels has been considered as a potential option for tissue engineering due to their physical and chemical characteristics. However, few studies associate the raw materials properties and processing conditions with the final characteristics of hydrogels, which could condition their use as scaffolds for tissue engineering. In this context, the main objective of this work was the evaluation of type I collagen as raw material for the elaboration of hydrogels. In addition, gelation time, pH and temperature were evaluated as the most influential variables in the hydrogel processing method by rheological (time, strain and frequency sweep tests) and microstructural (Cryo-SEM) measurements. The results indicate that it is possible to obtain collagen hydrogels with adequate rheological and microstructural characteristics by selecting optimal processing conditions. However, further studies are necessary to assess their suitability for cell accommodation and growth. Full article
(This article belongs to the Special Issue Functional Gelatin)
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21 pages, 3732 KiB  
Article
Inclusion of Cross-Linked Elastin in Gelatin/PEG Hydrogels Favourably Influences Fibroblast Phenotype
by Ye Cao, Bae Hoon Lee, Scott Alexander Irvine, Yee Shan Wong, Havazelet Bianco Peled and Subramanian Venkatraman
Polymers 2020, 12(3), 670; https://0-doi-org.brum.beds.ac.uk/10.3390/polym12030670 - 17 Mar 2020
Cited by 15 | Viewed by 5410
Abstract
The capacity of a biomaterial to innately modulate cell behavior while meeting the mechanical property requirements of the implant is a much sought-after goal within bioengineering. Here we covalently incorporate soluble elastin into a gelatin–poly (ethylene glycol) (PEG) hydrogel for three-dimensional (3D) cell [...] Read more.
The capacity of a biomaterial to innately modulate cell behavior while meeting the mechanical property requirements of the implant is a much sought-after goal within bioengineering. Here we covalently incorporate soluble elastin into a gelatin–poly (ethylene glycol) (PEG) hydrogel for three-dimensional (3D) cell encapsulation to achieve these properties. The inclusion of elastin into a previously optimized gelatin–PEG hydrogel was then evaluated for effects on entrapped fibroblasts, with the aim to assess the hydrogel as an extracellular matrix (ECM)-mimicking 3D microenvironment for cellular guidance. Soluble elastin was incorporated both physically and covalently into novel gelatin/elastin hybrid PEG hydrogels with the aim to harness the cellular interactivity and mechanical tunability of both elastin and gelatin. This design allowed us to assess the benefits of elastin-containing hydrogels in guiding fibroblast activity for evaluation as a potential dermal replacement. It was found that a gelatin–PEG hydrogel with covalently conjugated elastin, supported neonatal fibroblast viability, promoted their proliferation from 7.3% to 13.5% and guided their behavior. The expression of collagen alpha-1(COL1A1) and elastin in gelatin/elastin hybrid gels increased 16-fold and 6-fold compared to control sample at day 9, respectively. Moreover, cells can be loaded into the hydrogel precursor solution, deposited, and the matrix cross-linked without affecting the incorporated cells adversely, thus enabling a potential injectable system for dermal wound healing. Full article
(This article belongs to the Special Issue Functional Gelatin)
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11 pages, 1101 KiB  
Article
Effect of Fructose and Ascorbic Acid on the Performance of Cross-Linked Fish Gelatin Films
by Pedro Guerrero, Iraitz Zugasti, Alaitz Etxabide, Huynh Nguyen Duy Bao, Trung Trang Si, Miriam Peñalba and Koro de la Caba
Polymers 2020, 12(3), 570; https://0-doi-org.brum.beds.ac.uk/10.3390/polym12030570 - 04 Mar 2020
Cited by 11 | Viewed by 3232
Abstract
Gelatin was extracted from fish scales in this work, in an attempt to valorise abundant and available fishery by-products as an approach towards a more circular economy. With this strategy in mind, fish scale gelatin was used to prepare active films. In this [...] Read more.
Gelatin was extracted from fish scales in this work, in an attempt to valorise abundant and available fishery by-products as an approach towards a more circular economy. With this strategy in mind, fish scale gelatin was used to prepare active films. In this regard, the development of advanced materials from gelatin involves its modification to enhance functional properties, particularly barrier properties, to achieve the requirements for specific value-added purposes, such as food or pharmaceutical/biomedical applications. The improvement of those functional properties can be achieved by means of chemical cross-linking processes. In this context, non-enzymatic reactions were carried out with the addition of fructose and ascorbic acid into gelatin film forming formulations, and cross-linking was induced by a heat-treatment. These cross-linking reactions resulted in higher barrier features, especially for those films prepared with ascorbic acid. Full article
(This article belongs to the Special Issue Functional Gelatin)
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12 pages, 3294 KiB  
Article
The Effect of Cross-Linking with Citric Acid on the Properties of Agar/Fish Gelatin Films
by Jone Uranga, Bach T. Nguyen, Trung Trang Si, Pedro Guerrero and Koro de la Caba
Polymers 2020, 12(2), 291; https://0-doi-org.brum.beds.ac.uk/10.3390/polym12020291 - 02 Feb 2020
Cited by 50 | Viewed by 7712
Abstract
The aim of this work was to assess the effect of fish gelatin–citric acid nucleophilic substitution and agar–citric acid esterification reactions on the properties of agar/fish gelatin films. Since temperature is an important cross-linking parameter, films were treated at 90 °C and 105 [...] Read more.
The aim of this work was to assess the effect of fish gelatin–citric acid nucleophilic substitution and agar–citric acid esterification reactions on the properties of agar/fish gelatin films. Since temperature is an important cross-linking parameter, films were treated at 90 °C and 105 °C and film properties were compared to those of non-cured films. It was observed that temperature favored the aforementioned reactions, which induced physical and morphological changes. In this regard, darker films with a rougher surface were obtained for the films with a higher cross-linking degree. While mechanical properties were slightly modified, the barrier properties were enhanced due to the reactions that occurred. Therefore, these agar/fish gelatin films cross-linked through two different reactions can be considered to be promising materials as active films for different purposes, such as active packaging or pharmaceutical applications. Full article
(This article belongs to the Special Issue Functional Gelatin)
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11 pages, 3462 KiB  
Article
Cellular Orientation on Repeatedly Stretching Gelatin Hydrogels with Supramolecular Cross-Linkers
by Dae Hoon Lee, Yoshinori Arisaka, Asato Tonegawa, Tae Woong Kang, Atsushi Tamura and Nobuhiko Yui
Polymers 2019, 11(12), 2095; https://0-doi-org.brum.beds.ac.uk/10.3390/polym11122095 - 14 Dec 2019
Cited by 14 | Viewed by 3635
Abstract
The cytocompatibility of biological and synthetic materials is an important issue for biomaterials. Gelatin hydrogels are used as biomaterials because of their biodegradability. We have previously reported that the mechanical properties of gelatin hydrogels are improved by cross-linking with polyrotaxanes, a supramolecular compound [...] Read more.
The cytocompatibility of biological and synthetic materials is an important issue for biomaterials. Gelatin hydrogels are used as biomaterials because of their biodegradability. We have previously reported that the mechanical properties of gelatin hydrogels are improved by cross-linking with polyrotaxanes, a supramolecular compound composed of many cyclic molecules threaded with a linear polymer. In this study, the ability of gelatin hydrogels cross-linked by polyrotaxanes (polyrotaxane–gelatin hydrogels) for cell cultivation was investigated. Because the amount of polyrotaxanes used for gelatin fabrication is very small, the chemical composition was barely altered. The structure and wettability of these hydrogels are also the same as those of conventional hydrogels. Fibroblasts adhered on polyrotaxane–gelatin hydrogels and conventional hydrogels without any reduction or apoptosis of adherent cells. From these results, the polyrotaxane–gelatin hydrogels have the potential to improve the mechanical properties of gelatin without affecting cytocompatibility. Interestingly, when cells were cultured on polyrotaxane–gelatin hydrogels after repeated stress deformation, the cells were spontaneously oriented to the stretching direction. This cellular response was not observed on conventional hydrogels. These results suggest that the use of a polyrotaxane cross-linking agent can not only improve the strength of hydrogels but can also contribute to controlling reorientation of the gelatin. Full article
(This article belongs to the Special Issue Functional Gelatin)
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