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Biomedical Hydrogels: Synthesis and Applications

A special issue of Molecules (ISSN 1420-3049). This special issue belongs to the section "Materials Chemistry".

Deadline for manuscript submissions: closed (31 August 2020) | Viewed by 27735

Special Issue Editor


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Guest Editor
Department of Bioresources and Polymer Science, Faculty of Applied Chemistry and Materials Science, Politehnica University of Bucharest, Bucharest, Romania
Interests: hydrogels; thermosensitive polymers; terminally-reactive oligomers; controlled/living radical polymerization; block copolymers

Special Issue Information

Dear Colleagues,

Since their discovery by Lim and Wichterle in the early 1960s, hydrogels have evolved as a class of versatile materials with numerous uses in various fields like medicine and pharmacy, agriculture, cosmetics, personal hygiene, wastewater purification, and catalysis. Within the last decades, a multitude of hydrophilic (co)polymers, both naturally occurring and synthetic, have been researched in order to synthesize hydrogels for varied purposes, including controlled drug delivery systems, tissue regeneration and repair, biosensors or actuators, soil conditioners and agrochemicals slow delivery systems, catalysts, personal hygiene products, etc. Among them, the largest research effort has been directed toward biomedical hydrogel preparation, because of their water content making them similar to the human tissue correlated with the importance of human health. This Special Issue aims at gathering together new contributions discussing all aspects concerning the biomedical hydrogels, from synthesis to application, as either drug delivery and tissue engineering systems, biosensors, or contact lenses. Review articles by experts in the field are also welcome.

Prof. Dr. Mircea Teodorescu
Guest Editor

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Keywords

  • biomedical hydrogels
  • crosslinked hydrogels
  • injectable hydrogels
  • stimuli-sensitive hydrogels
  • biodegradable hydrogels
  • smart hydrogels
  • synthetic polymer hydrogels
  • naturally occurring polymer hydrogels
  • mixed hydrogels
  • (semi)interpenetrating network hydrogels
  • tissue engineering
  • drug delivery
  • biosensors
  • contact lenses

Published Papers (5 papers)

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Research

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14 pages, 3665 KiB  
Communication
The Effect of Ethanol on Gelation, Nanoscopic, and Macroscopic Properties of Serum Albumin Hydrogels
by Seyed Hamidreza Arabi, David Haselberger and Dariush Hinderberger
Molecules 2020, 25(8), 1927; https://0-doi-org.brum.beds.ac.uk/10.3390/molecules25081927 - 21 Apr 2020
Cited by 11 | Viewed by 2758
Abstract
Serum albumin has shown great potential in the development of new biomaterials for drug delivery systems. Different methods have been proposed to synthesis hydrogels out of serum albumin. It has been observed that ethanol can also act as a trigger for serum albumin [...] Read more.
Serum albumin has shown great potential in the development of new biomaterials for drug delivery systems. Different methods have been proposed to synthesis hydrogels out of serum albumin. It has been observed that ethanol can also act as a trigger for serum albumin denaturation and subsequent gelation. In this study, we focus on basic mechanisms of the albumin gelation process at 37 °C when using the chemical denaturant ethanol. The temperature of 37 °C was chosen to resemble human body temperature, and as under physiological conditions, albumin is in a non-denatured N conformation. As established in our previous publication for the triggers of pH and temperature (and time), we here explore the conformational and physical properties space of albumin hydrogels when they are ethanol-induced and show that the use of ethanol can be advisable for certain gel properties on the nanoscopic and macroscopic scale. To this end, we combine spectroscopic and mechanically (rheology) based data for characterizing the gels. We also study the gels′ binding capacities for fatty acids with electron paramagnetic resonance (EPR) spectroscopy, which implies observing the effects of bound stearic acids on gelation. Ethanol reduces the fraction of the strongly bound FAs in bovine serum albumin (BSA) hydrogels up to 52% and induces BSA hydrogels with a maximum storage modulus of 5000 Pa. The loosely bound FAs in ethanol-based hydrogels, besides their relatively weak mechanical properties, introduce interesting new materials for fast drug delivery systems and beyond. Full article
(This article belongs to the Special Issue Biomedical Hydrogels: Synthesis and Applications)
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20 pages, 14933 KiB  
Article
An Interpenetrating Alginate/Gelatin Network for Three-Dimensional (3D) Cell Cultures and Organ Bioprinting
by Qiuhong Chen, Xiaohong Tian, Jun Fan, Hao Tong, Qiang Ao and Xiaohong Wang
Molecules 2020, 25(3), 756; https://0-doi-org.brum.beds.ac.uk/10.3390/molecules25030756 - 10 Feb 2020
Cited by 48 | Viewed by 5930
Abstract
Crosslinking is an effective way to improve the physiochemical and biochemical properties of hydrogels. In this study, we describe an interpenetrating polymer network (IPN) of alginate/gelatin hydrogels (i.e., A-G-IPN) in which cells can be encapsulated for in vitro three-dimensional (3D) cultures and organ [...] Read more.
Crosslinking is an effective way to improve the physiochemical and biochemical properties of hydrogels. In this study, we describe an interpenetrating polymer network (IPN) of alginate/gelatin hydrogels (i.e., A-G-IPN) in which cells can be encapsulated for in vitro three-dimensional (3D) cultures and organ bioprinting. A double crosslinking model, i.e., using Ca2+ to crosslink alginate molecules and transglutaminase (TG) to crosslink gelatin molecules, is exploited to improve the physiochemical, such as water holding capacity, hardness and structural integrity, and biochemical properties, such as cytocompatibility, of the alginate/gelatin hydrogels. For the sake of convenience, the individual ionic (i.e., only treatment with Ca2+) or enzymatic (i.e., only treatment with TG) crosslinked alginate/gelatin hydrogels are referred as alginate-semi-IPN (i.e., A-semi-IPN) or gelatin-semi-IPN (i.e., G-semi-IPN), respectively. Tunable physiochemical and biochemical properties of the hydrogels have been obtained by changing the crosslinking sequences and polymer concentrations. Cytocompatibilities of the obtained hydrogels are evaluated through in vitro 3D cell cultures and bioprinting. The double crosslinked A-G-IPN hydrogel is a promising candidate for a wide range of biomedical applications, including bioartificial organ manufacturing, high-throughput drug screening, and pathological mechanism analyses. Full article
(This article belongs to the Special Issue Biomedical Hydrogels: Synthesis and Applications)
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13 pages, 2854 KiB  
Article
Development of RNA/DNA Hydrogel Targeting Toll-Like Receptor 7/8 for Sustained RNA Release and Potent Immune Activation
by Fusae Komura, Kana Okuzumi, Yuki Takahashi, Yoshinobu Takakura and Makiya Nishikawa
Molecules 2020, 25(3), 728; https://0-doi-org.brum.beds.ac.uk/10.3390/molecules25030728 - 07 Feb 2020
Cited by 23 | Viewed by 3653
Abstract
Guanosine- and uridine-rich single-stranded RNA (GU-rich RNA) is an agonist of Toll-like receptor (TLR) 7 and TLR8 and induces strong immune responses. A nanostructured GU-rich RNA/DNA assembly prepared using DNA nanotechnology can be used as an adjuvant capable of improving the biological stability [...] Read more.
Guanosine- and uridine-rich single-stranded RNA (GU-rich RNA) is an agonist of Toll-like receptor (TLR) 7 and TLR8 and induces strong immune responses. A nanostructured GU-rich RNA/DNA assembly prepared using DNA nanotechnology can be used as an adjuvant capable of improving the biological stability of RNA and promoting efficient RNA delivery to target immune cells. To achieve a sustained supply of GU-rich RNA to immune cells, we developed a GU-rich RNA/DNA hydrogel (RDgel) using nanostructured GU-rich RNA/DNA assembly, from which GU-rich RNA can be released in a sustained manner. A hexapod-like GU-rich RNA/DNA nanostructure, or hexapodRD6, was designed using a 20-mer phosphorothioate-stabilized GU-rich RNA and six phosphodiester DNAs. Two sets of hexapodRD6 were mixed to obtain RDgel. Under serum-containing conditions, GU-rich RNA was gradually released from the RDgel. Fluorescently labeled GU-rich RNA was efficiently taken up by DC2.4 murine dendritic cells and induced a high level of tumor necrosis factor-α release from these cells when it was incorporated into RDgel. These results indicate that the RDgel constructed using DNA nanotechnology can be a useful adjuvant in cancer therapy with sustained RNA release and high immunostimulatory activity. Full article
(This article belongs to the Special Issue Biomedical Hydrogels: Synthesis and Applications)
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14 pages, 3302 KiB  
Article
Design, Synthesis and Characterization of a Novel Type of Thermo-Responsible Phospholipid Microcapsule–Alginate Composite Hydrogel for Drug Delivery
by Liang Ding, Xinxia Cui, Rui Jiang, Keya Zhou, Yalei Wen, Chenfeng Wang, Zhilian Yue, Shigang Shen and Xuefeng Pan
Molecules 2020, 25(3), 694; https://0-doi-org.brum.beds.ac.uk/10.3390/molecules25030694 - 06 Feb 2020
Cited by 7 | Viewed by 4003
Abstract
Liposomes are extensively used in drug delivery, while alginates are widely used in tissue engineering. However, liposomes are usually thermally unstable and drug-leaking when in liquids, while the drug carriers made of alginates show low loading capacities when used for drug delivery. Herein, [...] Read more.
Liposomes are extensively used in drug delivery, while alginates are widely used in tissue engineering. However, liposomes are usually thermally unstable and drug-leaking when in liquids, while the drug carriers made of alginates show low loading capacities when used for drug delivery. Herein, we developed a type of thermo-responsible liposome–alginate composite hydrogel (TSPMAH) by grafting thermo-responsive liposomes onto alginates by using Ca2+ mediated bonding between the phosphatidic serine (PS) in the liposome membrane and the alginate. The temperature-sensitivity of the liposomes was actualized by using phospholipids comprising dipalmitoylphosphatidylcholine (DPPC) and PS and the liposomes were prepared by a thin-film dispersion method. The TSPMAH was then successfully prepared by bridge-linking the microcapsules onto the alginate hydrogel via PS-Ca2+-Carboxyl-alginate interaction. Characterizations of the TSPMAH were carried out using scanning electron microscopy, transform infrared spectroscopy, and laser scanning confocal microscopy, respectively. Their rheological property was also characterized by using a rheometer. Cytotoxicity evaluations of the TSPMAH showed that the composite hydrogel was biocompatible, safe, and non-toxic. Further, loading and thermos-inducible release of model drugs encapsulated by the TSPMAH as a drug carrier system was also studied by making protamine–siRNA complex-carrying TSPMAH drug carriers. Our results indicated that the TSPMAH described herein has great potentials to be further developed into an intelligent drug delivery system. Full article
(This article belongs to the Special Issue Biomedical Hydrogels: Synthesis and Applications)
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Review

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68 pages, 8926 KiB  
Review
New Developments in Medical Applications of Hybrid Hydrogels Containing Natural Polymers
by Cornelia Vasile, Daniela Pamfil, Elena Stoleru and Mihaela Baican
Molecules 2020, 25(7), 1539; https://0-doi-org.brum.beds.ac.uk/10.3390/molecules25071539 - 27 Mar 2020
Cited by 158 | Viewed by 10840
Abstract
New trends in biomedical applications of the hybrid polymeric hydrogels, obtained by combining natural polymers with synthetic ones, have been reviewed. Homopolysaccharides, heteropolysaccharides, as well as polypeptides, proteins and nucleic acids, are presented from the point of view of their ability to form [...] Read more.
New trends in biomedical applications of the hybrid polymeric hydrogels, obtained by combining natural polymers with synthetic ones, have been reviewed. Homopolysaccharides, heteropolysaccharides, as well as polypeptides, proteins and nucleic acids, are presented from the point of view of their ability to form hydrogels with synthetic polymers, the preparation procedures for polymeric organic hybrid hydrogels, general physico-chemical properties and main biomedical applications (i.e., tissue engineering, wound dressing, drug delivery, etc.). Full article
(This article belongs to the Special Issue Biomedical Hydrogels: Synthesis and Applications)
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