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Hydrogels in Regenerative Medicine and Other Biomedical Applications

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

Deadline for manuscript submissions: closed (15 November 2021) | Viewed by 71062

Printed Edition Available!
A printed edition of this Special Issue is available here.

Special Issue Editor

Dr. Peter John Jervis

E-Mail Website
Guest Editor
University of Minho, Braga, Portugal

Special Issue Information

Dear Colleagues,

I invite you and your research group to submit a research article to a Special Issue of the International Journal of Molecular Science titled “Hydrogels in Regenerative Medicine and Other Biomedical Applications”.

Great strides have been made in the area of hydrogel science since the first hydrogels were described in the 1960s. Hydrogels usually consist of three-dimensional matrices of hydrophilic polymers held together by chemical or physical crosslinks, or supramolecular assemblies of small amphiphilic molecules. The gelation process occurs in response to a physical or chemical stimulus, such as temperature, pH, electric or magnetic field, enzymatic modification, light, and others. Consisting of mainly water molecules, they represent a unique class of materials, with many applications such as cell therapeutics, cartilage/bone regeneration, sustained drug release and drug delivery systems, tissue engineering, and 3D bioprinting. Despite these great strides, there is still much more to discover in this area. This Special Issue is focused on the use of hydrogels in tissue and bone regeneration. Hydrogels are particularly suited for this purpose as their physical characteristics resemble that of the extracellular matrix, and as such they have found applications as an extracellular medium for cancer cells, stem cells, and neuronal cells. Research papers on the applications of hydrogels to other biomedical applications are also welcome. Due to the nature of this journal and its audience, publications should feature at least some discussion of the results on the molecular level.

Dr. Peter John Jervis
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. 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

  • soft materials
  • polymers
  • peptides
  • supramolecular
  • self-assembly
  • tissue regeneration
  • bone regeneration
  • wound healing
  • drug delivery
  • stimuli-responsive

Published Papers (18 papers)

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Editorial

Jump to: Research, Review

4 pages, 189 KiB  
Editorial
Hydrogels in Regenerative Medicine and Other Biomedical Applications
by Peter J. Jervis
Int. J. Mol. Sci. 2022, 23(6), 3270; https://doi.org/10.3390/ijms23063270 - 18 Mar 2022
Cited by 7 | Viewed by 1754
Abstract
It is my great pleasure to be part of this Special Issue in the International Journal of Molecular Sciences—“Hydrogels in Regenerative Medicine and Other Biomedical Applications” [...] Full article
(This article belongs to the Special Issue Hydrogels in Regenerative Medicine and Other Biomedical Applications)

Research

Jump to: Editorial, Review

12 pages, 4768 KiB  
Article
Injectable Human Hair Keratin–Fibrinogen Hydrogels for Engineering 3D Microenvironments to Accelerate Oral Tissue Regeneration
by Hyeon Jeong Kang, Nare Ko, Seung Jun Oh, Seong Yeong An, Yu-Shik Hwang and So Yeon Kim
Int. J. Mol. Sci. 2021, 22(24), 13269; https://doi.org/10.3390/ijms222413269 - 9 Dec 2021
Cited by 8 | Viewed by 2917
Abstract
Traumatic injury of the oral cavity is atypical and often accompanied by uncontrolled bleeding and inflammation. Injectable hydrogels have been considered to be promising candidates for the treatment of oral injuries because of their simple formulation, minimally invasive application technique, and site-specific delivery. [...] Read more.
Traumatic injury of the oral cavity is atypical and often accompanied by uncontrolled bleeding and inflammation. Injectable hydrogels have been considered to be promising candidates for the treatment of oral injuries because of their simple formulation, minimally invasive application technique, and site-specific delivery. Fibrinogen-based hydrogels have been widely explored as effective materials for wound healing in tissue engineering due to their uniqueness. Recently, an injectable foam has taken the spotlight. However, the fibrin component of this biomaterial is relatively stiff. To address these challenges, we created keratin-conjugated fibrinogen (KRT-FIB). This study aimed to develop a novel keratin biomaterial and assess cell–biomaterial interactions. Consequently, a novel injectable KRT-FIB hydrogel was optimized through rheological measurements, and its injection performance, swelling behavior, and surface morphology were investigated. We observed an excellent cell viability, proliferation, and migration/cell–cell interaction, indicating that the novel KRT-FIB-injectable hydrogel is a promising platform for oral tissue regeneration with a high clinical applicability. Full article
(This article belongs to the Special Issue Hydrogels in Regenerative Medicine and Other Biomedical Applications)
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23 pages, 6087 KiB  
Article
Development of Polyvinyl Alcohol/Kaolin Sponges Stimulated by Marjoram as Hemostatic, Antibacterial, and Antioxidant Dressings for Wound Healing Promotion
by Tamer M. Tamer, Mosa H. Alsehli, Ahmed M. Omer, Tarek H. Afifi, Maysa M. Sabet, Mohamed S. Mohy-Eldin and Mohamed A. Hassan
Int. J. Mol. Sci. 2021, 22(23), 13050; https://doi.org/10.3390/ijms222313050 - 2 Dec 2021
Cited by 43 | Viewed by 3472
Abstract
The predominant impediments to cutaneous wound regeneration are hemorrhage and bacterial infections that lead to extensive inflammation with lethal impact. We thus developed a series of composite sponges based on polyvinyl alcohol (PVA) inspired by marjoram essential oil and kaolin (PVA/marjoram/kaolin), adopting a [...] Read more.
The predominant impediments to cutaneous wound regeneration are hemorrhage and bacterial infections that lead to extensive inflammation with lethal impact. We thus developed a series of composite sponges based on polyvinyl alcohol (PVA) inspired by marjoram essential oil and kaolin (PVA/marjoram/kaolin), adopting a freeze–thaw method to treat irregular wounds by thwarting lethal bleeding and microbial infections. Microstructure analyses manifested three-dimensional interconnected porous structures for PVA/marjoram/kaolin. Additionally, upon increasing marjoram and kaolin concentrations, the pore diameters of the sponges significantly increased, recording a maximum of 34 ± 5.8 µm for PVA-M0.5-K0.1. Moreover, the porosity and degradation properties of PVA/marjoram/kaolin sponges were markedly enhanced compared with the PVA sponge with high swelling capacity. Furthermore, the PVA/marjoram/kaolin sponges exerted exceptional antibacterial performance against Escherichia coli and Bacillus cereus, along with remarkable antioxidant properties. Moreover, PVA/marjoram/kaolin sponges demonstrated significant thrombogenicity, developing high thrombus mass and hemocompatibility, in addition to their remarkable safety toward fibroblast cells. Notably, this is the first study to our knowledge investigating the effectiveness of marjoram in a polymeric carrier for prospective functioning as a wound dressing. Collectively, the findings suggest the prospective usage of the PVA-M0.5-K0.1 sponge in wound healing for hemorrhage and bacterial infection control. Full article
(This article belongs to the Special Issue Hydrogels in Regenerative Medicine and Other Biomedical Applications)
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12 pages, 4680 KiB  
Article
Ultrasound Imaging by Thermally Tunable Phononic Crystal Lens
by Yuqi Jin and Arup Neogi
Int. J. Mol. Sci. 2021, 22(15), 7966; https://doi.org/10.3390/ijms22157966 - 26 Jul 2021
Cited by 5 | Viewed by 1994
Abstract
This work demonstrates the detections and mappings of a solid object using a thermally tunable solid-state phononic crystal lens at low frequency for potential use in future long-distance detection. The phononic crystal lens is infiltrated with a polyvinyl alcohol-based poly n-isopropyl acrylamide (PVA-PNIPAm) [...] Read more.
This work demonstrates the detections and mappings of a solid object using a thermally tunable solid-state phononic crystal lens at low frequency for potential use in future long-distance detection. The phononic crystal lens is infiltrated with a polyvinyl alcohol-based poly n-isopropyl acrylamide (PVA-PNIPAm) bulk hydrogel polymer. The hydrogel undergoes a volumetric phase transition due to a temperature change leading to a temperature-dependent sound velocity and density. The temperature variation from 20 °C to 39 °C changes the focal length of the tunable solid-state lens by 1 cm in the axial direction. This thermo-reversible tunable focal length lens was used in a monostatic setup for one- and two-dimensional mapping scans in both frequency domain echo-intensity and temporal domain time-of-flight modes. The experimental results illustrated 1.03 ± 0.15λ and 2.35 ± 0.28λ on the lateral and axial minimum detectable object size. The experiments using the tunable lens demonstrate the capability to detect objects by changing the temperature in water without translating an object, source, or detector. The time-of-flight mode modality using the tunable solid-state phononic lens increases the signal-to-noise ratio compared to a conventional phononic crystal lens. Full article
(This article belongs to the Special Issue Hydrogels in Regenerative Medicine and Other Biomedical Applications)
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18 pages, 6328 KiB  
Article
Bio-Functionalized Chitosan for Bone Tissue Engineering
by Paola Brun, Annj Zamuner, Chiara Battocchio, Leonardo Cassari, Martina Todesco, Valerio Graziani, Giovanna Iucci, Martina Marsotto, Luca Tortora, Valeria Secchi and Monica Dettin
Int. J. Mol. Sci. 2021, 22(11), 5916; https://doi.org/10.3390/ijms22115916 - 31 May 2021
Cited by 32 | Viewed by 3917
Abstract
Hybrid biomaterials allow for the improvement of the biological properties of materials and have been successfully used for implantology in medical applications. The covalent and selective functionalization of materials with bioactive peptides provides favorable results in tissue engineering by supporting cell attachment to [...] Read more.
Hybrid biomaterials allow for the improvement of the biological properties of materials and have been successfully used for implantology in medical applications. The covalent and selective functionalization of materials with bioactive peptides provides favorable results in tissue engineering by supporting cell attachment to the biomaterial through biochemical cues and interaction with membrane receptors. Since the functionalization with bioactive peptides may alter the chemical and physical properties of the biomaterials, in this study we characterized the biological responses of differently functionalized chitosan analogs. Chitosan analogs were produced through the reaction of GRGDSPK (RGD) or FRHRNRKGY (HVP) sequences, both carrying an aldehyde-terminal group, to chitosan. The bio-functionalized polysaccharides, pure or “diluted” with chitosan, were chemically characterized in depth and evaluated for their antimicrobial activities and biocompatibility toward human primary osteoblast cells. The results obtained indicate that the bio-functionalization of chitosan increases human-osteoblast adhesion (p < 0.005) and proliferation (p < 0.005) as compared with chitosan. Overall, the 1:1 mixture of HVP functionalized-chitosan:chitosan is the best compromise between preserving the antibacterial properties of the material and supporting osteoblast differentiation and calcium deposition (p < 0.005 vs. RGD). In conclusion, our results reported that a selected concentration of HVP supported the biomimetic potential of functionalized chitosan better than RGD and preserved the antibacterial properties of chitosan. Full article
(This article belongs to the Special Issue Hydrogels in Regenerative Medicine and Other Biomedical Applications)
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17 pages, 4104 KiB  
Article
Accelerated and Improved Vascular Maturity after Transplantation of Testicular Tissue in Hydrogels Supplemented with VEGF- and PDGF-Loaded Nanoparticles
by Federico Del Vento, Jonathan Poels, Maxime Vermeulen, Bernard Ucakar, Maria Grazia Giudice, Marc Kanbar, Anne des Rieux and Christine Wyns
Int. J. Mol. Sci. 2021, 22(11), 5779; https://doi.org/10.3390/ijms22115779 - 28 May 2021
Cited by 19 | Viewed by 2545
Abstract
Avascular transplantation of frozen–thawed testicular tissue fragments represents a potential future technique for fertility restoration in boys with cancer. A significant loss of spermatogonia was observed in xeno-transplants of human tissue most likely due to the hypoxic period before revascularization. To reduce the [...] Read more.
Avascular transplantation of frozen–thawed testicular tissue fragments represents a potential future technique for fertility restoration in boys with cancer. A significant loss of spermatogonia was observed in xeno-transplants of human tissue most likely due to the hypoxic period before revascularization. To reduce the effect of hypoxia–reoxygenation injuries, several options have already been explored, like encapsulation in alginate hydrogel and supplementation with nanoparticles delivering a necrosis inhibitor (NECINH) or VEGF. While these approaches improved short-term (5 days) vascular surfaces in grafts, neovessels were not maintained up to 21 days; i.e., the time needed for achieving vessel stabilization. To better support tissue grafts, nanoparticles loaded with VEGF, PDGF and NECINH were developed. Testicular tissue fragments from 4–5-week-old mice were encapsulated in calcium-alginate hydrogels, either non-supplemented (control) or supplemented with drug-loaded nanoparticles (VEGF-nanoparticles; VEGF-nanoparticles + PDGF-nanoparticles; NECINH-nanoparticles; VEGF-nanoparticles + NECINH-nanoparticles; and VEGF-nanoparticles + PDGF-nanoparticles + NECINH-nanoparticles) before auto-transplantation. Grafts were recovered after 5 or 21 days for analyses of tissue integrity (hematoxylin–eosin staining), spermatogonial survival (immuno-histo-chemistry for promyelocytic leukemia zinc finger) and vascularization (immuno-histo-chemistry for α-smooth muscle actin and CD-31). Our results showed that a combination of VEGF and PDGF nanoparticles increased vascular maturity and induced a faster maturation of vascular structures in grafts. Full article
(This article belongs to the Special Issue Hydrogels in Regenerative Medicine and Other Biomedical Applications)
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17 pages, 3447 KiB  
Article
Synthesis and Evaluation of AlgNa-g-Poly(QCL-co-HEMA) Hydrogels as Platform for Chondrocyte Proliferation and Controlled Release of Betamethasone
by Jomarien García-Couce, Marioly Vernhes, Nancy Bada, Lissette Agüero, Oscar Valdés, José Alvarez-Barreto, Gastón Fuentes, Amisel Almirall and Luis J. Cruz
Int. J. Mol. Sci. 2021, 22(11), 5730; https://doi.org/10.3390/ijms22115730 - 27 May 2021
Cited by 14 | Viewed by 3237
Abstract
Hydrogels obtained from combining different polymers are an interesting strategy for developing controlled release system platforms and tissue engineering scaffolds. In this study, the applicability of sodium alginate-g-(QCL-co-HEMA) hydrogels for these biomedical applications was evaluated. Hydrogels were synthesized by free-radical polymerization using a [...] Read more.
Hydrogels obtained from combining different polymers are an interesting strategy for developing controlled release system platforms and tissue engineering scaffolds. In this study, the applicability of sodium alginate-g-(QCL-co-HEMA) hydrogels for these biomedical applications was evaluated. Hydrogels were synthesized by free-radical polymerization using a different concentration of the components. The hydrogels were characterized by Fourier transform-infrared spectroscopy, scanning electron microscopy, and a swelling degree. Betamethasone release as well as the in vitro cytocompatibility with chondrocytes and fibroblast cells were also evaluated. Scanning electron microscopy confirmed the porous surface morphology of the hydrogels in all cases. The swelling percent was determined at a different pH and was observed to be pH-sensitive. The controlled release behavior of betamethasone from the matrices was investigated in PBS media (pH = 7.4) and the drug was released in a controlled manner for up to 8 h. Human chondrocytes and fibroblasts were cultured on the hydrogels. The MTS assay showed that almost all hydrogels are cytocompatibles and an increase of proliferation in both cell types after one week of incubation was observed by the Live/Dead® assay. These results demonstrate that these hydrogels are attractive materials for pharmaceutical and biomedical applications due to their characteristics, their release kinetics, and biocompatibility. Full article
(This article belongs to the Special Issue Hydrogels in Regenerative Medicine and Other Biomedical Applications)
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18 pages, 13313 KiB  
Article
Bioprinting Via a Dual-Gel Bioink Based on Poly(Vinyl Alcohol) and Solubilized Extracellular Matrix towards Cartilage Engineering
by Mohsen Setayeshmehr, Shahzad Hafeez, Clemens van Blitterswijk, Lorenzo Moroni, Carlos Mota and Matthew B. Baker
Int. J. Mol. Sci. 2021, 22(8), 3901; https://doi.org/10.3390/ijms22083901 - 9 Apr 2021
Cited by 25 | Viewed by 3285
Abstract
Various hydrogel systems have been developed as biomaterial inks for bioprinting, including natural and synthetic polymers. However, the available biomaterial inks, which allow printability, cell viability, and user-defined customization, remains limited. Incorporation of biological extracellular matrix materials into tunable synthetic polymers can merge [...] Read more.
Various hydrogel systems have been developed as biomaterial inks for bioprinting, including natural and synthetic polymers. However, the available biomaterial inks, which allow printability, cell viability, and user-defined customization, remains limited. Incorporation of biological extracellular matrix materials into tunable synthetic polymers can merge the benefits of both systems towards versatile materials for biofabrication. The aim of this study was to develop novel, cell compatible dual-component biomaterial inks and bioinks based on poly(vinyl alcohol) (PVA) and solubilized decellularized cartilage matrix (SDCM) hydrogels that can be utilized for cartilage bioprinting. In a first approach, PVA was modified with amine groups (PVA-A), and mixed with SDCM. The printability of the PVA-A/SDCM formulations cross-linked by genipin was evaluated. On the second approach, the PVA was functionalized with cis-5-norbornene-endo-2,3-dicarboxylic anhydride (PVA-Nb) to allow an ultrafast light-curing thiol-ene cross-linking. Comprehensive experiments were conducted to evaluate the influence of the SDCM ratio in mechanical properties, water uptake, swelling, cell viability, and printability of the PVA-based formulations. The studies performed with the PVA-A/SDCM formulations cross-linked by genipin showed printability, but poor shape retention due to slow cross-linking kinetics. On the other hand, the PVA-Nb/SDCM showed good printability. The results showed that incorporation of SDCM into PVA-Nb reduces the compression modulus, enhance cell viability, and bioprintability and modulate the swelling ratio of the resulted hydrogels. Results indicated that PVA-Nb hydrogels containing SDCM could be considered as versatile bioinks for cartilage bioprinting. Full article
(This article belongs to the Special Issue Hydrogels in Regenerative Medicine and Other Biomedical Applications)
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19 pages, 4508 KiB  
Article
Alginate-g-PNIPAM-Based Thermo/Shear-Responsive Injectable Hydrogels: Tailoring the Rheological Properties by Adjusting the LCST of the Grafting Chains
by Konstantinos Safakas, Sofia-Falia Saravanou, Zacharoula Iatridi and Constantinos Tsitsilianis
Int. J. Mol. Sci. 2021, 22(8), 3824; https://doi.org/10.3390/ijms22083824 - 7 Apr 2021
Cited by 20 | Viewed by 3311
Abstract
Graft copolymers of alginate backbone and N-isopropylacrylamide/N-tert-butylacrylamide random copolymer, P(NIPAMx-co-NtBAMy), side chains (stickers) with various NtBAM content were designed and explored in aqueous media. Self-assembling thermoresponsive hydrogels are formed upon heating, in all cases, [...] Read more.
Graft copolymers of alginate backbone and N-isopropylacrylamide/N-tert-butylacrylamide random copolymer, P(NIPAMx-co-NtBAMy), side chains (stickers) with various NtBAM content were designed and explored in aqueous media. Self-assembling thermoresponsive hydrogels are formed upon heating, in all cases, through the hydrophobic association of the P(NIPAMx-co-NtBAMy) sticky pendant chains. The rheological properties of the formulations depend remarkably on the NtBAM hydrophobic content, which regulates the lower critical solution temperature (LCST) and, in turn, the stickers’ thermo-responsiveness. The gelation point, Tgel, was shifted to lower temperatures from 38 to 20 °C by enriching the PNIPAM chains with 20 mol % NtBAM, shifting accordingly to the gelation temperature window. The consequences of the Tgel shift to the hydrogels’ rheological properties are significant at room and body temperature. For instance, at 37 °C, the storage modulus increases about two orders of magnitude and the terminal relaxation time increase about 10 orders of magnitude by enriching the stickers with 20 mol % hydrophobic moieties. Two main thermo-induced behaviors were revealed, characterized by a sol–gel and a weak gel–stiff gel transition for the copolymer with stickers of low (0.6 mol %) and high (14, 20 mol %) NtBAM content, respectively. The first type of hydrogels is easily injectable, while for the second one, the injectability is provided by shear-thinning effects. The influence of the type of media (phosphate buffer (PB), phosphate-buffered saline (PBS), Dulbecco’s modified Eagle’s medium (DMEM)) on the hydrogel properties was also explored and discussed. The 4 wt % NaALG-g-P(NIPAM80-co-NtBAM20)/DMEM formulation showed excellent shear-induced injectability at room temperature and instantaneous thermo-induced gel stiffening at body temperature, rendering it a good candidate for cell transplantation potential applications. Full article
(This article belongs to the Special Issue Hydrogels in Regenerative Medicine and Other Biomedical Applications)
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11 pages, 3540 KiB  
Article
Pathogenic Hydrogel? A Novel-Entrapment Neuropathy Model Induced by Ultrasound-Guided Perineural Injections
by Ming-Yen Hsiao, Ya-Wen Wu, Wen-Shiang Chen, Yu-Ling Lin, Po-Ling Kuo and Chueh-Hung Wu
Int. J. Mol. Sci. 2021, 22(7), 3494; https://doi.org/10.3390/ijms22073494 - 28 Mar 2021
Cited by 1 | Viewed by 2773
Abstract
Entrapment neuropathy (EN) is a prevalent and debilitative condition caused by a complex pathogenesis that involves a chronic compression–edema–ischemia cascade and perineural adhesion that results in excessive shear stress during motion. Despite decades of research, an easily accessible and surgery-free animal model mimicking [...] Read more.
Entrapment neuropathy (EN) is a prevalent and debilitative condition caused by a complex pathogenesis that involves a chronic compression–edema–ischemia cascade and perineural adhesion that results in excessive shear stress during motion. Despite decades of research, an easily accessible and surgery-free animal model mimicking the mixed etiology is currently lacking, thus limiting our understanding of the disease and the development of effective therapies. In this proof-of-concept study, we used ultrasound-guided perineural injection of a methoxy poly(ethylene glycol)-b-Poly(lactide-co-glycoilide) carboxylic acid (mPEG-PLGA-BOX) hydrogel near the rat’s sciatic nerve to induce EN, as confirmed sonographically, electrophysiologically, and histologically. The nerve that was injected with hydrogel appeared unevenly contoured and swollen proximally with slowed nerve conduction velocities across the injected segments, thus showing the compressive features of EN. Histology showed perineural cellular infiltration, deposition of irregular collagen fibers, and a possible early demyelination process, thus indicating the existence of adhesions. The novel method provides a surgery-free and cost-effective way to establish a small-animal model of EN that has mixed compression and adhesion features, thus facilitating the additional elucidation of the pathophysiology of EN and the search for promising treatments. Full article
(This article belongs to the Special Issue Hydrogels in Regenerative Medicine and Other Biomedical Applications)
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22 pages, 7388 KiB  
Article
Enhanced Regeneration of Vascularized Adipose Tissue with Dual 3D-Printed Elastic Polymer/dECM Hydrogel Complex
by Soojin Lee, Hyun Su Lee, Justin J. Chung, Soo Hyun Kim, Jong Woong Park, Kangwon Lee and Youngmee Jung
Int. J. Mol. Sci. 2021, 22(6), 2886; https://doi.org/10.3390/ijms22062886 - 12 Mar 2021
Cited by 22 | Viewed by 3569
Abstract
A flexible and bioactive scaffold for adipose tissue engineering was fabricated and evaluated by dual nozzle three-dimensional printing. A highly elastic poly (L-lactide-co-ε-caprolactone) (PLCL) copolymer, which acted as the main scaffolding, and human adipose tissue derived decellularized extracellular matrix (dECM) hydrogels were used [...] Read more.
A flexible and bioactive scaffold for adipose tissue engineering was fabricated and evaluated by dual nozzle three-dimensional printing. A highly elastic poly (L-lactide-co-ε-caprolactone) (PLCL) copolymer, which acted as the main scaffolding, and human adipose tissue derived decellularized extracellular matrix (dECM) hydrogels were used as the printing inks to form the scaffolds. To prepare the three-dimensional (3D) scaffolds, the PLCL co-polymer was printed with a hot melting extruder system while retaining its physical character, similar to adipose tissue, which is beneficial for regeneration. Moreover, to promote adipogenic differentiation and angiogenesis, adipose tissue-derived dECM was used. To optimize the printability of the hydrogel inks, a mixture of collagen type I and dECM hydrogels was used. Furthermore, we examined the adipose tissue formation and angiogenesis of the PLCL/dECM complex scaffold. From in vivo experiments, it was observed that the matured adipose-like tissue structures were abundant, and the number of matured capillaries was remarkably higher in the hydrogel–PLCL group than in the PLCL-only group. Moreover, a higher expression of M2 macrophages, which are known to be involved in the remodeling and regeneration of tissues, was detected in the hydrogel–PLCL group by immunofluorescence analysis. Based on these results, we suggest that our PLCL/dECM fabricated by a dual 3D printing system will be useful for the treatment of large volume fat tissue regeneration. Full article
(This article belongs to the Special Issue Hydrogels in Regenerative Medicine and Other Biomedical Applications)
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19 pages, 18591 KiB  
Article
Heparin-Mimicking Polymer-Based In Vitro Platform Recapitulates In Vivo Muscle Atrophy Phenotypes
by Hyunbum Kim, Ji Hoon Jeong, Mona Fendereski, Hyo-Shin Lee, Da Yeon Kang, Sung Sik Hur, Jhaleh Amirian, Yunhye Kim, Nghia Thi Pham, Nayoung Suh, Nathaniel Suk-Yeon Hwang, Seongho Ryu, Jeong Kyo Yoon and Yongsung Hwang
Int. J. Mol. Sci. 2021, 22(5), 2488; https://doi.org/10.3390/ijms22052488 - 2 Mar 2021
Cited by 6 | Viewed by 3064
Abstract
The cell–cell/cell–matrix interactions between myoblasts and their extracellular microenvironment have been shown to play a crucial role in the regulation of in vitro myogenic differentiation and in vivo skeletal muscle regeneration. In this study, by harnessing the heparin-mimicking polymer, poly(sodium-4-styrenesulfonate) (PSS), which has [...] Read more.
The cell–cell/cell–matrix interactions between myoblasts and their extracellular microenvironment have been shown to play a crucial role in the regulation of in vitro myogenic differentiation and in vivo skeletal muscle regeneration. In this study, by harnessing the heparin-mimicking polymer, poly(sodium-4-styrenesulfonate) (PSS), which has a negatively charged surface, we engineered an in vitro cell culture platform for the purpose of recapitulating in vivo muscle atrophy-like phenotypes. Our initial findings showed that heparin-mimicking moieties inhibited the fusion of mononucleated myoblasts into multinucleated myotubes, as indicated by the decreased gene and protein expression levels of myogenic factors, myotube fusion-related markers, and focal adhesion kinase (FAK). We further elucidated the underlying molecular mechanism via transcriptome analyses, observing that the insulin/PI3K/mTOR and Wnt signaling pathways were significantly downregulated by heparin-mimicking moieties through the inhibition of FAK/Cav3. Taken together, the easy-to-adapt heparin-mimicking polymer-based in vitro cell culture platform could be an attractive platform for potential applications in drug screening, providing clear readouts of changes in insulin/PI3K/mTOR and Wnt signaling pathways. Full article
(This article belongs to the Special Issue Hydrogels in Regenerative Medicine and Other Biomedical Applications)
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17 pages, 2586 KiB  
Article
RGDS-Modified Superporous Poly(2-Hydroxyethyl Methacrylate)-Based Scaffolds as 3D In Vitro Leukemia Model
by Hana Svozilová, Zdeněk Plichta, Vladimír Proks, Radana Studená, Jiří Baloun, Michael Doubek, Šárka Pospíšilová and Daniel Horák
Int. J. Mol. Sci. 2021, 22(5), 2376; https://doi.org/10.3390/ijms22052376 - 27 Feb 2021
Cited by 9 | Viewed by 2566
Abstract
Superporous poly(2-hydroxyethyl methacrylate-co-2-aminoethyl methacrylate) (P(HEMA-AEMA)) hydrogel scaffolds are designed for in vitro 3D culturing of leukemic B cells. Hydrogel porosity, which influences cell functions and growth, is introduced by adding ammonium oxalate needle-like crystals in the polymerization mixture. To improve cell [...] Read more.
Superporous poly(2-hydroxyethyl methacrylate-co-2-aminoethyl methacrylate) (P(HEMA-AEMA)) hydrogel scaffolds are designed for in vitro 3D culturing of leukemic B cells. Hydrogel porosity, which influences cell functions and growth, is introduced by adding ammonium oxalate needle-like crystals in the polymerization mixture. To improve cell vitality, cell-adhesive Arg-Gly-Asp-Ser (RGDS) peptide is immobilized on the N-(γ-maleimidobutyryloxy)succinimide-activated P(HEMA-AEMA) hydrogels via reaction of SH with maleimide groups. This modification is especially suitable for the survival of primary chronic lymphocytic leukemia cells (B-CLLs) in 3D cell culture. No other tested stimuli (interleukin-4, CD40 ligand, or shaking) can further improve B-CLL survival or metabolic activity. Both unmodified and RGDS-modified P(HEMA-AEMA) scaffolds serve as a long-term (70 days) 3D culture platforms for HS-5 and M2-10B4 bone marrow stromal cell lines and MEC-1 and HG-3 B-CLL cell lines, although the adherent cells retain their physiological morphologies, preferably on RGDS-modified hydrogels. Moreover, the porosity of hydrogels allows direct cell lysis, followed by efficient DNA isolation from the 3D-cultured cells. P(HEMA-AEMA)-RGDS thus serves as a suitable 3D in vitro leukemia model that enables molecular and metabolic assays and allows imaging of cell morphology, interactions, and migration by confocal microscopy. Such applications can prospectively assist in testing of drugs to treat this frequently recurring or refractory cancer. Full article
(This article belongs to the Special Issue Hydrogels in Regenerative Medicine and Other Biomedical Applications)
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16 pages, 6346 KiB  
Article
β-Cyclodextrin/Triclosan Complex-Grafted Methacrylated Glycol Chitosan Hydorgel by Photocrosslinking via Visible Light Irradiation for a Tissue Bio-Adhesive
by Young Jae Moon, Sun-Jung Yoon, Jeung-Hyun Koo, Yihyun Yoon, Hye Jun Byun, Hyeon Soo Kim, Gilson Khang, Heung Jae Chun and Dae Hyeok Yang
Int. J. Mol. Sci. 2021, 22(2), 700; https://doi.org/10.3390/ijms22020700 - 12 Jan 2021
Cited by 12 | Viewed by 5260
Abstract
Accelerating wound healing with minimized bacterial infection has become a topic of interest in the development of the new generation of tissue bio-adhesives. In this study, we fabricated a hydrogel system (MGC-g-CD-ic-TCS) consisting of triclosan (TCS)-complexed beta-cyclodextrin (β-CD)-conjugated methacrylated glycol chitosan (MGC) as [...] Read more.
Accelerating wound healing with minimized bacterial infection has become a topic of interest in the development of the new generation of tissue bio-adhesives. In this study, we fabricated a hydrogel system (MGC-g-CD-ic-TCS) consisting of triclosan (TCS)-complexed beta-cyclodextrin (β-CD)-conjugated methacrylated glycol chitosan (MGC) as an antibacterial tissue adhesive. Proton nuclear magnetic resonance (1H NMR) and differential scanning calorimetry (DSC) results showed the inclusion complex formation between MGC-g-CD and TCS. The increase of storage modulus (G’) of MGC-g-CD-ic-TCS after visible light irradiation for 200 s indicated its hydrogelation. The swollen hydrogel in aqueous solution resulted in two release behaviors of an initial burst and sustained release. Importantly, in vitro and in vivo results indicated that MGC-g-CD-ic-TCS inhibited bacterial infection and improved wound healing, suggesting its high potential application as an antibacterial tissue bio-adhesive. Full article
(This article belongs to the Special Issue Hydrogels in Regenerative Medicine and Other Biomedical Applications)
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15 pages, 3599 KiB  
Article
Evaluation of Polyvinyl Alcohol/Cobalt Substituted Hydroxyapatite Nanocomposite as a Potential Wound Dressing for Diabetic Foot Ulcers
by Wei-Chun Lin and Cheng-Ming Tang
Int. J. Mol. Sci. 2020, 21(22), 8831; https://doi.org/10.3390/ijms21228831 - 22 Nov 2020
Cited by 14 | Viewed by 3415
Abstract
Diabetic foot ulcers (DFUs) caused by diabetes are prone to serious and persistent infections. If not treated properly, it will cause tissue necrosis or septicemia due to peripheral blood vessel embolism. Therefore, it is an urgent challenge to accelerate wound healing and reduce [...] Read more.
Diabetic foot ulcers (DFUs) caused by diabetes are prone to serious and persistent infections. If not treated properly, it will cause tissue necrosis or septicemia due to peripheral blood vessel embolism. Therefore, it is an urgent challenge to accelerate wound healing and reduce the risk of bacterial infection in patients. In clinical practice, DFUs mostly use hydrogel dressing to cover the surface of the affected area as an auxiliary treatment. Polyvinyl alcohol (PVA) is a hydrophilic hydrogel polymer widely used in dressings, drug delivery, and medical applications. However, due to its weak bioactivity and antibacterial ability, leads to limited application. Filler adding is a useful way to enhance the biocompatibility of PVA. In our study, cobalt-substituted hydroxyapatite (CoHA) powder was prepared by the electrochemically-deposited method. PVA and PVA-CoHA nanocomposite were prepared by the solvent casting method. The bioactivity of the PVA and composite was evaluated by immersed in simulated body fluid for 7 days. In addition, L929 cells and E. coli were used to evaluate the cytotoxicity and antibacterial tests of PVA and PVA-CoHA nanocomposite. The results show that the addition of CoHA increases the mechanical properties and biological activity of PVA. Biocompatibility evaluation showed no significant cytotoxicity of PVA-CoHA composite. In addition, a small amount of cobalt ion was released to the culture medium from the nanocomposite in the cell culture period and enhanced cell growth. The addition of CoHA also confirmed that it could inhibit the growth of E. coli. PVA-CoHA composite may have potential applications in diabetic trauma healing and wound dressing. Full article
(This article belongs to the Special Issue Hydrogels in Regenerative Medicine and Other Biomedical Applications)
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Review

Jump to: Editorial, Research

48 pages, 19157 KiB  
Review
Engineering Hydrogels for the Development of Three-Dimensional In Vitro Models
by Somnath Maji and Hyungseok Lee
Int. J. Mol. Sci. 2022, 23(5), 2662; https://doi.org/10.3390/ijms23052662 - 28 Feb 2022
Cited by 24 | Viewed by 5420
Abstract
The superiority of in vitro 3D cultures over conventional 2D cell cultures is well recognized by the scientific community for its relevance in mimicking the native tissue architecture and functionality. The recent paradigm shift in the field of tissue engineering toward the development [...] Read more.
The superiority of in vitro 3D cultures over conventional 2D cell cultures is well recognized by the scientific community for its relevance in mimicking the native tissue architecture and functionality. The recent paradigm shift in the field of tissue engineering toward the development of 3D in vitro models can be realized with its myriad of applications, including drug screening, developing alternative diagnostics, and regenerative medicine. Hydrogels are considered the most suitable biomaterial for developing an in vitro model owing to their similarity in features to the extracellular microenvironment of native tissue. In this review article, recent progress in the use of hydrogel-based biomaterial for the development of 3D in vitro biomimetic tissue models is highlighted. Discussions of hydrogel sources and the latest hybrid system with different combinations of biopolymers are also presented. The hydrogel crosslinking mechanism and design consideration are summarized, followed by different types of available hydrogel module systems along with recent microfabrication technologies. We also present the latest developments in engineering hydrogel-based 3D in vitro models targeting specific tissues. Finally, we discuss the challenges surrounding current in vitro platforms and 3D models in the light of future perspectives for an improved biomimetic in vitro organ system. Full article
(This article belongs to the Special Issue Hydrogels in Regenerative Medicine and Other Biomedical Applications)
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19 pages, 2562 KiB  
Review
Dehydropeptide Supramolecular Hydrogels and Nanostructures as Potential Peptidomimetic Biomedical Materials
by Peter J. Jervis, Carolina Amorim, Teresa Pereira, José A. Martins and Paula M. T. Ferreira
Int. J. Mol. Sci. 2021, 22(5), 2528; https://doi.org/10.3390/ijms22052528 - 3 Mar 2021
Cited by 13 | Viewed by 3293
Abstract
Supramolecular peptide hydrogels are gaining increased attention, owing to their potential in a variety of biomedical applications. Their physical properties are similar to those of the extracellular matrix (ECM), which is key to their applications in the cell culture of specialized cells, tissue [...] Read more.
Supramolecular peptide hydrogels are gaining increased attention, owing to their potential in a variety of biomedical applications. Their physical properties are similar to those of the extracellular matrix (ECM), which is key to their applications in the cell culture of specialized cells, tissue engineering, skin regeneration, and wound healing. The structure of these hydrogels usually consists of a di- or tripeptide capped on the N-terminus with a hydrophobic aromatic group, such as Fmoc or naphthalene. Although these peptide conjugates can offer advantages over other types of gelators such as cross-linked polymers, they usually possess the limitation of being particularly sensitive to proteolysis by endogenous proteases. One of the strategies reported that can overcome this barrier is to use a peptidomimetic strategy, in which natural amino acids are switched for non-proteinogenic analogues, such as D-amino acids, β-amino acids, or dehydroamino acids. Such peptides usually possess much greater resistance to enzymatic hydrolysis. Peptides containing dehydroamino acids, i.e., dehydropeptides, are particularly interesting, as the presence of the double bond also introduces a conformational restraint to the peptide backbone, resulting in (often predictable) changes to the secondary structure of the peptide. This review focuses on peptide hydrogels and related nanostructures, where α,β-didehydro-α-amino acids have been successfully incorporated into the structure of peptide hydrogelators, and the resulting properties are discussed in terms of their potential biomedical applications. Where appropriate, their properties are compared with those of the corresponding peptide hydrogelator composed of canonical amino acids. In a wider context, we consider the presence of dehydroamino acids in natural compounds and medicinally important compounds as well as their limitations, and we consider some of the synthetic strategies for obtaining dehydropeptides. Finally, we consider the future direction for this research area. Full article
(This article belongs to the Special Issue Hydrogels in Regenerative Medicine and Other Biomedical Applications)
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30 pages, 1471 KiB  
Review
Chitosan and Cellulose-Based Hydrogels for Wound Management
by Sibusiso Alven and Blessing Atim Aderibigbe
Int. J. Mol. Sci. 2020, 21(24), 9656; https://doi.org/10.3390/ijms21249656 - 18 Dec 2020
Cited by 160 | Viewed by 13536
Abstract
Wound management remains a challenge worldwide, although there are several developed wound dressing materials for the management of acute and chronic wounds. The wound dressings that are currently used include hydrogels, films, wafers, nanofibers, foams, topical formulations, transdermal patches, sponges, and bandages. Hydrogels [...] Read more.
Wound management remains a challenge worldwide, although there are several developed wound dressing materials for the management of acute and chronic wounds. The wound dressings that are currently used include hydrogels, films, wafers, nanofibers, foams, topical formulations, transdermal patches, sponges, and bandages. Hydrogels exhibit unique features which make them suitable wound dressings such as providing a moist environment for wound healing, exhibiting high moisture content, or creating a barrier against bacterial infections, and are suitable for the management of exuding and granulating wounds. Biopolymers have been utilized for their development due to their non-toxic, biodegradable, and biocompatible properties. Hydrogels have been prepared from biopolymers such as cellulose and chitosan by crosslinking with selected synthetic polymers resulting in improved mechanical, biological, and physicochemical properties. They were useful by accelerating wound re-epithelialization and also mimic skin structure, inducing skin regeneration. Loading antibacterial agents into them prevented bacterial invasion of wounds. This review article is focused on hydrogels formulated from two biopolymers—chitosan and cellulose—for improved wound management. Full article
(This article belongs to the Special Issue Hydrogels in Regenerative Medicine and Other Biomedical Applications)
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