Hydrogelated Matrices: Structural, Functional and Applicative Aspects

A special issue of Gels (ISSN 2310-2861). This special issue belongs to the section "Gel Chemistry and Physics".

Deadline for manuscript submissions: closed (15 October 2024) | Viewed by 29518

Special Issue Editors


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Guest Editor
IRCCS Synlab SDN, Via G. Ferraris 144, 80146 Naples, Italy
Interests: hydrogels; nanogels; bioactive peptides; peptides as diagnostic and therapeutics; supramolecular chemistry; diagnostic and drug delivery technologies; material characterization; nanomedicine
Special Issues, Collections and Topics in MDPI journals

E-Mail Website
Guest Editor
1. Department of Pharmacy, Via Domenico Montesano 49, 80131 Naples, Italy
2. Research Centre on Bioactive Peptides (CIRPeB), University of Naples “Federico II”, 80134 Naples, Italy
Interests: peptide self-assembling; peptide-based materials; amyloid materials; hydrogels; fibers; material characterization; co-assembly
Special Issues, Collections and Topics in MDPI journals

Special Issue Information

Dear Colleagues,

In collaboration with Dr. Carlo Diaferia, we are glad to announce the Special Issue of Gels titled “Hydrogelated Matrices: Structural, Functional and Applicative Aspects”. Generated by multi-scale organization, hydro-, aero- and organogelated matrices are soft materials that are useful for horizon applications. Formed by both polymers or self-assembling molecules via non-covalent interactions or through supramolecular chemistry pathways, these materials were identified as useful tools for exploring different areas of application, including sustained API (active pharmaceutical ingredient) delivery, tissue engineering, optoelectronics, sensors and surface modification. In addition to the increased interest regarding their functional properties, the chemical and physical forces that promote the gelation process have received extensive attention. Furthermore, the handling of these materials allows their existence in multiple forms, including injectable formulations, films, thin coatings and nanocomposites. This Special Issue aims to enhance the knowledge about the structural, organizational and applicative features of the gels’ state of matter. Full research articles, reviews, letters and mini reviews that cover these topics or similar topics are welcome.

Dr. Enrico Gallo
Dr. Carlo Diaferia
Guest Editors

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Keywords

  • hydrogelated matrices
  • supramolecular aggregates
  • peptide-based aggregates
  • hydrogels formulation and characterization
  • nanogels formulation and characterization
  • nanofibers
  • multicomponent gels
  • organogels
  • soft materials
  • biotechnological applications
  • supramolecular agents for bioimaging
  • active pharmaceutical ingredient (API) delivery
  • surfaces and coating

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Published Papers (15 papers)

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Research

22 pages, 5499 KiB  
Article
Development of Polyvinyl Alcohol Hydrogels for Controlled Glucose Release in Biomedical Applications
by Rosa M. Quispe-Siccha, Osvaldo I. Medina-Sandoval, Abraham Estrada-Tinoco, Jorge A. Pedroza-Pérez, Adolfo Martínez-Tovar, Irma Olarte-Carrillo, Rafael Cerón-Maldonado, Arturo Reding-Bernal and Juan C. López-Alvarenga
Gels 2024, 10(10), 668; https://doi.org/10.3390/gels10100668 - 19 Oct 2024
Viewed by 1001
Abstract
Polyvinyl alcohol (PVA) hydrogels have a wide range of applications in the pharmaceutical and biomedicine fields due to their exceptional biophysical properties. The study focuses on preparing and characterizing capsule-shaped PVA hydrogels to enhance their biocompatibility and porosity for controlled glucose release and [...] Read more.
Polyvinyl alcohol (PVA) hydrogels have a wide range of applications in the pharmaceutical and biomedicine fields due to their exceptional biophysical properties. The study focuses on preparing and characterizing capsule-shaped PVA hydrogels to enhance their biocompatibility and porosity for controlled glucose release and cell proliferation. The hydrogels were prepared using different concentrations (Cs) and molecular weights (MWs) of PVA, with two different lengths, A (10 mm) and B (20 mm), to control glucose release over 60 min. The preparation process involved PVA gel preparation and PVA hydrogel formation. A total of 500 µL of glucose was injected into all dehydrated hydrogels in groups A and B. Glucose release was studied by immersing the hydrogels in saline at 37 °C with stirring at 500 rpm. The SUP-B15 cell line was grown in six A1 hydrogels for biocompatibility testing. The results indicate that all hydrogels remained stable at 37 °C without degrading. Those with a higher C and MW exhibited a denser and less porous structure, lower glucose storage capacity, and higher elongation at break. Significant differences in glucose release, diffusion speed, and flux were observed, which were more evident in A1 > A4, B1 > B4, and B1 > A1 over 60 min. A1 and B1 had higher values because their higher porosity distribution allowed glucose to diffuse more easily. B1, being larger, has more glucose due to its increased length. The cell growth response and viability at 48 h in contact with the hydrogels was similar to that of the control (4.5 × 105 cells/mL, 98.5% vs. 4.8 × 105 cells/mL, 99.7% viability), thus demonstrating biocompatibility. The hydrogels effectively released glucose over 60 min, with variations based on porosity, C, MW, and length, and demonstrated good biocompatibility with the cell line. Full article
(This article belongs to the Special Issue Hydrogelated Matrices: Structural, Functional and Applicative Aspects)
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20 pages, 12251 KiB  
Article
In Situ Gelling Behavior and Biopharmaceutical Characterization of Nano-Silver-Loaded Poloxamer Matrices Designed for Nasal Drug Delivery
by Nadezhda Ivanova, Neli Ermenlieva, Lora Simeonova, Neli Vilhelmova-Ilieva, Kameliya Bratoeva, Georgi Stoyanov and Velichka Andonova
Gels 2024, 10(6), 385; https://doi.org/10.3390/gels10060385 - 5 Jun 2024
Cited by 1 | Viewed by 1232
Abstract
A combination of Poloxamer 407 (P407) and hydroxypropyl methylcellulose (HPMC) hydrosols is proposed as an in situ thermo-gelling vehicle for the nasal drug delivery of chlorhexidine–silver nanoparticles conjugates (SN-CX). Optimization of the formulation was carried out by applying varying ratios of P407 and [...] Read more.
A combination of Poloxamer 407 (P407) and hydroxypropyl methylcellulose (HPMC) hydrosols is proposed as an in situ thermo-gelling vehicle for the nasal drug delivery of chlorhexidine–silver nanoparticles conjugates (SN-CX). Optimization of the formulation was carried out by applying varying ratios of P407 and HPMC in the presence and absence of SN-CX so that gelation would occur in the temperature range of the nasal cavity (30–34 °C). Mechanisms for the observed gelation phenomena were suggested based on viscosimetry, texture analysis, and dynamic light scattering. Tests were carried out for sprayability, washout time, in vitro drug release, ex vivo permeation, and antimicrobial activity. When applied separately, HPMC was found to lower the P407 gelation temperature (Tg), whereas SN-CX increased it. However, in the presence of HPMC, SN-CX interfered with the P407 micellar organization in a principally contrasting way while leading to an even further decrease in Tg. SN-CX-loaded nasal formulations composed of P407 16% and HPMC 0.1% demonstrated a desired gelation at 31.9 °C, good sprayability (52.95% coverage of the anterior nasal cavity), mucoadhesion for 70 min under simulated nasal clearance, expedient release and permeation, and preserved anti-infective activity against seasonal Influenza virus and beta-coronavirus, Pseudomonas aeruginosa, Klebsiella pneumoniae, Staphylococcus aureus and other pathogens. Our findings suggest that the current development could be considered a potential formulation of a protective nasal spray against respiratory infections. Full article
(This article belongs to the Special Issue Hydrogelated Matrices: Structural, Functional and Applicative Aspects)
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16 pages, 9226 KiB  
Article
Ag0–Ginger Nanocomposites Integrated into Natural Hydrogelated Matrices Used as Antimicrobial Delivery Systems Deposited on Cellulose Fabrics
by Florentina Monica Raduly, Valentin Raditoiu, Alina Raditoiu, Maria Grapin, Mariana Constantin, Iuliana Răut, Cristian Andi Nicolae and Adriana Nicoleta Frone
Gels 2024, 10(2), 106; https://doi.org/10.3390/gels10020106 - 27 Jan 2024
Cited by 1 | Viewed by 1878
Abstract
In the textile, medical, and food industries, many of the applications have targeted the use of textile fabrics with antimicrobial properties. Obtaining eco-friendly coatings is of wide interest, especially for applications related to wound dressing or to food packaging. In order to obtain [...] Read more.
In the textile, medical, and food industries, many of the applications have targeted the use of textile fabrics with antimicrobial properties. Obtaining eco-friendly coatings is of wide interest, especially for applications related to wound dressing or to food packaging. In order to obtain coatings with antimicrobial properties through environmentally friendly methods, a series of experiments were carried out on the use of natural polymers loaded with silver nanoparticles. In this study, coatings with antimicrobial properties were obtained by depositing natural composites based on rice flour, carob flour, or alginate on cotton fabrics. These antimicrobial coatings were multicomponent systems, in which the host matrix was generated via hydration of natural polymers. The nanocomposite obtained from the phytosynthesis of silver particles in ginger extract was embedded in hydrogel matrices. The multicomponent gels obtained by embedding silver nanoparticles in natural polymer matrices were deposited on cotton fabric and were studied in relation to nanoparticles and the type of host matrix, and the antimicrobial activity was evaluated. Fabrics coated with such systems provide a hydrophilic surface with antimicrobial properties and can therefore be used in various areas where textiles provide antibacterial protection. Full article
(This article belongs to the Special Issue Hydrogelated Matrices: Structural, Functional and Applicative Aspects)
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22 pages, 5525 KiB  
Article
Self-Assembly of a Novel Pentapeptide into Hydrogelated Dendritic Architecture: Synthesis, Properties, Molecular Docking and Prospective Applications
by Stefania-Claudia Jitaru, Andra-Cristina Enache, Corneliu Cojocaru, Gabi Drochioiu, Brindusa-Alina Petre and Vasile-Robert Gradinaru
Gels 2024, 10(2), 86; https://doi.org/10.3390/gels10020086 - 23 Jan 2024
Cited by 1 | Viewed by 2011
Abstract
Currently, ultrashort oligopeptides consisting of fewer than eight amino acids represent a cutting-edge frontier in materials science, particularly in the realm of hydrogel formation. By employing solid-phase synthesis with the Fmoc/tBu approach, a novel pentapeptide, FEYNF-NH2, was designed, inspired by a [...] Read more.
Currently, ultrashort oligopeptides consisting of fewer than eight amino acids represent a cutting-edge frontier in materials science, particularly in the realm of hydrogel formation. By employing solid-phase synthesis with the Fmoc/tBu approach, a novel pentapeptide, FEYNF-NH2, was designed, inspired by a previously studied sequence chosen from hen egg-white lysozyme (FESNF-NH2). Qualitative peptide analysis was based on reverse-phase high performance liquid chromatography (RP-HPLC), while further purification was accomplished using solid-phase extraction (SPE). Exact molecular ion confirmation was achieved by matrix-assisted laser desorption–ionization mass spectrometry (MALDI-ToF MS) using two different matrices (HCCA and DHB). Additionally, the molecular ion of interest was subjected to tandem mass spectrometry (MS/MS) employing collision-induced dissociation (CID) to confirm the synthesized peptide structure. A combination of research techniques, including Fourier-transform infrared spectroscopy (FTIR), fluorescence analysis, transmission electron microscopy, polarized light microscopy, and Congo red staining assay, were carefully employed to glean valuable insights into the self-assembly phenomena and gelation process of the modified FEYNF-NH2 peptide. Furthermore, molecular docking simulations were conducted to deepen our understanding of the mechanisms underlying the pentapeptide’s supramolecular assembly formation and intermolecular interactions. Our study provides potential insights into amyloid research and proposes a novel peptide for advancements in materials science. In this regard, in silico studies were performed to explore the FEYNF peptide’s ability to form polyplexes. Full article
(This article belongs to the Special Issue Hydrogelated Matrices: Structural, Functional and Applicative Aspects)
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17 pages, 4201 KiB  
Article
Ultrashort Cationic Peptide Fmoc-FFK as Hydrogel Building Block for Potential Biomedical Applications
by Enrico Gallo, Carlo Diaferia, Sabrina Giordano, Elisabetta Rosa, Barbara Carrese, Gennaro Piccialli, Nicola Borbone, Giancarlo Morelli, Giorgia Oliviero and Antonella Accardo
Gels 2024, 10(1), 12; https://doi.org/10.3390/gels10010012 - 22 Dec 2023
Viewed by 2077
Abstract
Fmoc-diphenylalanine (Fmoc-FF) is a low-molecular-weight peptide hydrogelator. This simple all-aromatic peptide can generate self-supporting hydrogel materials, which have been proposed as novel materials for diagnostic and pharmaceutical applications. Our knowledge of the molecular determinants of Fmoc-FF aggregation is used as a guide to [...] Read more.
Fmoc-diphenylalanine (Fmoc-FF) is a low-molecular-weight peptide hydrogelator. This simple all-aromatic peptide can generate self-supporting hydrogel materials, which have been proposed as novel materials for diagnostic and pharmaceutical applications. Our knowledge of the molecular determinants of Fmoc-FF aggregation is used as a guide to design new peptide-based gelators, with features for the development of improved tools. Here, we enlarge the plethora of Fmoc-FF-based hydrogelated matrices by studying the properties of the Fmoc-FFK tripeptide, alone or in combination with Fmoc-FF. For multicomponent matrices, the relative weight ratios between Fmoc-FFK and Fmoc-FF (specifically, 1/1, 1/5, 1/10, and 1/20 w/w) are evaluated. All the systems and their multiscale organization are studied using different experimental techniques, including rheology, circular dichroism, Fourier transform infrared spectroscopy, and scanning electron microscopy (SEM). Preliminary profiles of biocompatibility for the studied systems are also described by testing them in vitro on HaCaT and 3T3-L1 cell lines. Additionally, the lysine (K) residue at the C-terminus of the Fmoc-FF moiety introduces into the supramolecular material chemical functions (amino groups) which may be useful for modification/derivatization with bioactive molecules of interest, including diagnostic probes, chelating agents, active pharmaceutical ingredients, or peptide nucleic acids. Full article
(This article belongs to the Special Issue Hydrogelated Matrices: Structural, Functional and Applicative Aspects)
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10 pages, 726 KiB  
Article
Akkermansia muciniphila Encapsulated in Calcium-Alginate Hydrogelated Matrix: Viability and Stability over Aerobic Storage and Simulated Gastrointestinal Conditions
by Daniela Machado, Mariana Fonseca, Rita Vedor, Sérgio Sousa, Joana Cristina Barbosa and Ana Maria Gomes
Gels 2023, 9(11), 869; https://doi.org/10.3390/gels9110869 - 1 Nov 2023
Cited by 3 | Viewed by 1925
Abstract
Akkermansia muciniphila is considered a next-generation probiotic to be incorporated in new food and pharmaceutical formulations. Effective delivery systems are required to ensure high probiotic viability and stability during product manufacture, shelf-life, and post-consumption, namely, throughout digestion. Hydrogelated matrices have demonstrated promising potential in [...] Read more.
Akkermansia muciniphila is considered a next-generation probiotic to be incorporated in new food and pharmaceutical formulations. Effective delivery systems are required to ensure high probiotic viability and stability during product manufacture, shelf-life, and post-consumption, namely, throughout digestion. Hydrogelated matrices have demonstrated promising potential in this dominion. Hence, this work aimed to evaluate the effect of a calcium-alginate hydrogelated matrix on A. muciniphila viability during 28-days refrigerated aerobic storage and when exposed to simulated gastrointestinal conditions, in comparison with that of free cells. Akkermansia muciniphila was successfully encapsulated in the calcium-alginate matrix via extrusion (60% encapsulation yield). Furthermore, encapsulated A. muciniphila exhibited high stability (a loss in viability lower than 0.2 log-cycle) after 28-days of refrigerated aerobic storage, maintaining its viability around 108 CFU/g. Prominently, as the storage time increased, encapsulated A. muciniphila revealed higher viability and stability regarding in vitro gastrointestinal conditions than free cells. This suggests that this encapsulation method may attenuate the detrimental effects of prolonged aerobic storage with a subsequent gastrointestinal passage. In conclusion, encapsulation via extrusion using a calcium-alginate hydrogelated matrix seems to be a promising and adequate strategy for safeguarding A. muciniphila from adverse conditions encountered during refrigerated aerobic storage and when exposed to the gastrointestinal passage. Full article
(This article belongs to the Special Issue Hydrogelated Matrices: Structural, Functional and Applicative Aspects)
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18 pages, 13376 KiB  
Article
Thermosensitive Hydrogel-Functionalized Mesoporous Silica Nanoparticles for Parenteral Application of Chemotherapeutics
by Christina Voycheva, Marta Slavkova, Teodora Popova, Diana Tzankova, Denitsa Stefanova, Virginia Tzankova, Ivelina Ivanova, Stanislav Tzankov, Ivanka Spassova, Daniela Kovacheva and Borislav Tzankov
Gels 2023, 9(9), 769; https://doi.org/10.3390/gels9090769 - 21 Sep 2023
Cited by 5 | Viewed by 1678
Abstract
Hydrogels can offer many opportunities for drug delivery strategies. They can be used on their own, or their benefits can be further exploited in combination with other nanocarriers. Intelligent hydrogels that react to changes in the surrounding environment can be utilized as gatekeepers [...] Read more.
Hydrogels can offer many opportunities for drug delivery strategies. They can be used on their own, or their benefits can be further exploited in combination with other nanocarriers. Intelligent hydrogels that react to changes in the surrounding environment can be utilized as gatekeepers and provide sustained on-demand drug release. In this study, a hybrid nanosystem for temperature- and pH-sensitive delivery was prepared from MCM-41 nanoparticles grafted with a newly synthesized thermosensitive hydrogel (MCM-41/AA-g-PnVCL). The initial particles were chemically modified by the attachment of carboxyl groups. Later, they were grafted with agar (AA) and vinylcaprolactam (VCL) by free radical polymerization. Doxorubicin was applied as a model hydrophilic chemotherapeutic drug. The successful formulation was confirmed by FT-IR and TGA. Transmission electron microscopy and dynamic light scattering analysis showed small particles with negative zeta potential. Their release behaviour was investigated in vitro in media with different pH and at different temperatures. Under tumour simulating conditions (40 °C and pH 4.0), doxorubicin was almost completely released within 72 h. The biocompatibility of the proposed nanoparticles was demonstrated by in vitro haemolysis assay. These results suggest the possible parenteral application of the newly prepared hydrogel-functionalized mesoporous silica nanoparticles for temperature-sensitive and pH-triggered drug delivery at the tumour site. Full article
(This article belongs to the Special Issue Hydrogelated Matrices: Structural, Functional and Applicative Aspects)
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20 pages, 3123 KiB  
Article
Modification of Acorn Starch Structure and Properties by High Hydrostatic Pressure
by Luís M. G. Castro, Ana I. Caço, Carla F. Pereira, Sérgio C. Sousa, María E. Brassesco, Manuela Machado, Óscar L. Ramos, Elisabete M. C. Alexandre, Jorge A. Saraiva and Manuela Pintado
Gels 2023, 9(9), 757; https://doi.org/10.3390/gels9090757 - 17 Sep 2023
Viewed by 1449
Abstract
Despite being rich in starch, over half of acorn production is undervalued. High hydrostatic pressure was used to modify the properties of Q. pyrenaica (0.1 and 460 MPa for 20 min) and Q. robur (0.1 and 333 MPa for 17.4 min) acorn starches [...] Read more.
Despite being rich in starch, over half of acorn production is undervalued. High hydrostatic pressure was used to modify the properties of Q. pyrenaica (0.1 and 460 MPa for 20 min) and Q. robur (0.1 and 333 MPa for 17.4 min) acorn starches to obtain high-valued ingredients. Pressure significantly altered the span distribution and heterogeneity of the acorn starch granules depending on the species, but their morphology was unaffected. Pressurization increased the amylose/amylopectin ratio and damaged starch contents, but the effect was more prominent in Q. pyrenaica than in Q. robur. However, the polymorphism, relative crystallinity, gelatinization temperatures, and enthalpies were preserved. The pressure effect on the starch properties depended on the property and species. The solubility, swelling power, and acorn gels’ resistance towards deformation for both species decreased after pressurization. For Q. pyrenaica starch, the in vitro digestibility increased, but the pseudoplastic behavior decreased after pressurization. No differences were seen for Q. robur. Regarding the commercial starch, acorn starches had lower gelatinization temperatures and enthalpies, lower in vitro digestibility, lower resistance towards deformation, superior pseudoplastic behavior, and overall higher solubility and swelling power until 80 °C. This encourages the usage of acorn starches as a new food ingredient. Full article
(This article belongs to the Special Issue Hydrogelated Matrices: Structural, Functional and Applicative Aspects)
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21 pages, 6254 KiB  
Article
Study of Polyvinyl Alcohol Hydrogels Applying Physical-Mechanical Methods and Dynamic Models of Photoacoustic Signals
by Roberto G. Ramírez-Chavarría, Argelia Pérez-Pacheco, Emiliano Terán and Rosa M. Quispe-Siccha
Gels 2023, 9(9), 727; https://doi.org/10.3390/gels9090727 - 7 Sep 2023
Cited by 1 | Viewed by 1472
Abstract
This study aims to analyze the physical-mechanical properties and dynamic models of tissue-simulating hydrogels, specifically the photoacoustic (PA) response signals, by varying the concentrations of polyvinyl alcohol (PVA) and molecular weight (MW). A state-space model (SSM) is proposed to study the PVA hydrogels [...] Read more.
This study aims to analyze the physical-mechanical properties and dynamic models of tissue-simulating hydrogels, specifically the photoacoustic (PA) response signals, by varying the concentrations of polyvinyl alcohol (PVA) and molecular weight (MW). A state-space model (SSM) is proposed to study the PVA hydrogels to retrieve the PA-related signal’s damping ratio and natural frequency. Nine box-shaped PVA hydrogels containing saline solution were used, with five concentrations of PVA (7, 9, 12, 15, 20%) for MW1 and four for MW2. The results indicated that the concentration of PVA and MW played an important role in the PA wave’s amplitude, arrival time, and speed of sound over the hydrogels. The SSM parameters showed that increasing PVA and MW concentrations improved the hydrogels’ ability to absorb and transfer energy under the PA effect. These parameters were also found to be correlated with density and modulus of elasticity. Additionally, the concentrations of PVA and MW affected the absorption and optical scattering coefficients. The physical-mechanical properties, including porosity, density, and modulus of elasticity, improved as the concentration of PVA and MW increased. The ultimate goal of this study is to develop hydrogels as phantoms that can be used for tissue simulation and imaging. Full article
(This article belongs to the Special Issue Hydrogelated Matrices: Structural, Functional and Applicative Aspects)
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13 pages, 3492 KiB  
Article
3D Co-Printing and Substrate Geometry Influence the Differentiation of C2C12 Skeletal Myoblasts
by Giada Loi, Franca Scocozza, Flaminia Aliberti, Lorenza Rinvenuto, Gianluca Cidonio, Nicola Marchesi, Laura Benedetti, Gabriele Ceccarelli and Michele Conti
Gels 2023, 9(7), 595; https://doi.org/10.3390/gels9070595 - 24 Jul 2023
Cited by 2 | Viewed by 2005
Abstract
Cells are influenced by several biomechanical aspects of their microenvironment, such as substrate geometry. According to the literature, substrate geometry influences the behavior of muscle cells; in particular, the curvature feature improves cell proliferation. However, the effect of substrate geometry on the myogenic [...] Read more.
Cells are influenced by several biomechanical aspects of their microenvironment, such as substrate geometry. According to the literature, substrate geometry influences the behavior of muscle cells; in particular, the curvature feature improves cell proliferation. However, the effect of substrate geometry on the myogenic differentiation process is not clear and needs to be further investigated. Here, we show that the 3D co-printing technique allows the realization of substrates. To test the influence of the co-printing technique on cellular behavior, we realized linear polycaprolactone substrates with channels in which a fibrinogen-based hydrogel loaded with C2C12 cells was deposited. Cell viability and differentiation were investigated up to 21 days in culture. The results suggest that this technology significantly improves the differentiation at 14 days. Therefore, we investigate the substrate geometry influence by comparing three different co-printed geometries—linear, circular, and hybrid structures (linear and circular features combined). Based on our results, all structures exhibit optimal cell viability (>94%), but the linear pattern allows to increase the in vitro cell differentiation, in particular after 14 days of culture. This study proposes an endorsed approach for creating artificial muscles for future skeletal muscle tissue engineering applications. Full article
(This article belongs to the Special Issue Hydrogelated Matrices: Structural, Functional and Applicative Aspects)
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12 pages, 3671 KiB  
Article
Cross-Linked Gel Polymer Electrolyte Based on Multiple Epoxy Groups Enabling Conductivity and High Performance of Li-Ion Batteries
by Wei Zhang, Wansu Bae, Lei Jin, Sungjun Park, Minhyuk Jeon, Whangi Kim and Hohyoun Jang
Gels 2023, 9(5), 384; https://doi.org/10.3390/gels9050384 - 5 May 2023
Viewed by 2106
Abstract
The low ionic conductivity and unstable interface of electrolytes/electrodes are the key issues hindering the application progress of lithium-ion batteries (LiBs). In this work, a cross-linked gel polymer electrolyte (C-GPE) based on epoxidized soybean oil (ESO) was synthesized by in situ thermal polymerization [...] Read more.
The low ionic conductivity and unstable interface of electrolytes/electrodes are the key issues hindering the application progress of lithium-ion batteries (LiBs). In this work, a cross-linked gel polymer electrolyte (C-GPE) based on epoxidized soybean oil (ESO) was synthesized by in situ thermal polymerization using lithium bis(fluorosulfonyl)imide (LiFSI) as an initiator. Ethylene carbonate/diethylene carbonate (EC/DEC) was beneficial for the distribution of the as-prepared C-GPE on the anode surface and the dissociation ability of LiFSI. The resulting C-GPE-2 exhibited a wide electrochemical window (of up to 5.19 V vs. Li+/Li), an ionic conductivity (σ) of 0.23 × 10−3 S/cm at 30 °C, a super-low glass transition temperature (Tg), and good interfacial stability between the electrodes and electrolyte. The battery performance of the as-prepared C-GPE-2 based on a graphite/LiFePO4 cell showed a high specific capacity of ca. 161.3 mAh/g (an initial Coulombic efficiency (CE) of ca. 98.4%) with a capacity retention rate of ca. 98.5% after 50 cycles at 0.1 C and an average CE of about ca. 98.04% at an operating voltage range of 2.0~4.2 V. This work provides a reference for designing cross-linking gel polymer electrolytes with high ionic conductivity, facilitating the practical application of high-performance LiBs. Full article
(This article belongs to the Special Issue Hydrogelated Matrices: Structural, Functional and Applicative Aspects)
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21 pages, 5783 KiB  
Article
Magnetic Ionotropic Hydrogels Based on Carboxymethyl Cellulose for Aqueous Pollution Mitigation
by Andra-Cristina Enache, Ionela Grecu, Petrisor Samoila, Corneliu Cojocaru and Valeria Harabagiu
Gels 2023, 9(5), 358; https://doi.org/10.3390/gels9050358 - 24 Apr 2023
Cited by 6 | Viewed by 1838
Abstract
In this work, stabilized ionotropic hydrogels were designed using sodium carboxymethyl cellulose (CMC) and assessed as inexpensive sorbents for hazardous chemicals (e.g., Methylene Blue, MB) from contaminated wastewaters. In order to increase the adsorption capacity of the hydrogelated matrix and facilitate its magnetic [...] Read more.
In this work, stabilized ionotropic hydrogels were designed using sodium carboxymethyl cellulose (CMC) and assessed as inexpensive sorbents for hazardous chemicals (e.g., Methylene Blue, MB) from contaminated wastewaters. In order to increase the adsorption capacity of the hydrogelated matrix and facilitate its magnetic separation from aqueous solutions, sodium dodecyl sulfate (SDS) and manganese ferrite (MnFe2O4) were introduced into the polymer framework. The morphological, structural, elemental, and magnetic properties of the adsorbents (in the form of beads) were assessed using scanning electron microscopy (SEM), energy-dispersive X-ray analysis, Fourier-transform infrared spectroscopy (FTIR), and a vibrating-sample magnetometer (VSM). The magnetic beads with the best adsorption performance were subjected to kinetic and isotherm studies. The PFO model best describes the adsorption kinetics. A homogeneous monolayer adsorption system was predicted by the Langmuir isotherm model, registering a maximum adsorption capacity of 234 mg/g at 300 K. The calculated thermodynamic parameter values indicated that the investigated adsorption processes were both spontaneous (ΔG < 0) and exothermic (ΔH < 0). The used sorbent can be recovered after immersion in acetone (93% desorption efficiency) and re-used for MB adsorption. In addition, the molecular docking simulations disclosed aspects of the mechanism of intermolecular interaction between CMC and MB by detailing the contributions of the van der Waals (physical) and Coulomb (electrostatic) forces. Full article
(This article belongs to the Special Issue Hydrogelated Matrices: Structural, Functional and Applicative Aspects)
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16 pages, 7637 KiB  
Article
A Light Scattering Investigation of Enzymatic Gelation in Self-Assembling Peptides
by Stefano Buzzaccaro, Vincenzo Ruzzi, Fabrizio Gelain and Roberto Piazza
Gels 2023, 9(4), 347; https://doi.org/10.3390/gels9040347 - 19 Apr 2023
Cited by 2 | Viewed by 1677
Abstract
Self-assembling peptides (SAPs) have been increasingly studied as hydrogel–former gelators because they can create biocompatible environments. A common strategy to trigger gelation, is to use a pH variation, but most methods result in a change in pH that is too rapid, leading to [...] Read more.
Self-assembling peptides (SAPs) have been increasingly studied as hydrogel–former gelators because they can create biocompatible environments. A common strategy to trigger gelation, is to use a pH variation, but most methods result in a change in pH that is too rapid, leading to gels with hardly reproducible properties. Here, we use the urea–urease reaction to tune gel properties, by a slow and uniform pH increase. We were able to produce very homogeneous and transparent gels at several SAP concentrations, ranging from c=1g/L to c=10g/L. In addition, by exploiting such a pH control strategy, and combining photon correlation imaging with dynamic light scattering measurements, we managed to unravel the mechanism by which gelation occurs in solutions of (LDLK)3-based SAPs. We found that, in diluted and concentrated solutions, gelation follows different pathways. This leads to gels with different microscopic dynamics and capability of trapping nanoparticles. At high concentrations, a strong gel is formed, made of relatively thick and rigid branches that firmly entrap nanoparticles. By contrast, the gel formed in dilute conditions is weaker, characterized by entanglements and crosslinks of very thin and flexible filaments. The gel is still able to entrap nanoparticles, but their motion is not completely arrested. These different gel morphologies can potentially be exploited for controlled multiple drug release. Full article
(This article belongs to the Special Issue Hydrogelated Matrices: Structural, Functional and Applicative Aspects)
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11 pages, 2620 KiB  
Article
Tumor Microenvironment-Responsive 6-Mercaptopurine-Releasing Injectable Hydrogel for Colon Cancer Treatment
by Sungjun Kim, Wonjeong Lee, Heewon Park and Kyobum Kim
Gels 2023, 9(4), 319; https://doi.org/10.3390/gels9040319 - 10 Apr 2023
Cited by 3 | Viewed by 2467
Abstract
Colon cancer is a significant health concern. The development of effective drug delivery systems is critical for improving treatment outcomes. In this study, we developed a drug delivery system for colon cancer treatment by embedding 6-mercaptopurine (6-MP), an anticancer drug, in a thiolated [...] Read more.
Colon cancer is a significant health concern. The development of effective drug delivery systems is critical for improving treatment outcomes. In this study, we developed a drug delivery system for colon cancer treatment by embedding 6-mercaptopurine (6-MP), an anticancer drug, in a thiolated gelatin/polyethylene glycol diacrylate hydrogel (6MP-GPGel). The 6MP-GPGel continuously released 6-MP, the anticancer drug. The release rate of 6-MP was further accelerated in an acidic or glutathione environment that mimicked a tumor microenvironment. In addition, when pure 6-MP was used for treatment, cancer cells proliferated again from day 5, whereas a continuous supply of 6-MP from the 6MP-GPGel continuously suppressed the survival rate of cancer cells. In conclusion, our study demonstrates that embedding 6-MP in a hydrogel formulation can improve the efficacy of colon cancer treatment and may serve as a promising minimally invasive and localized drug delivery system for future development. Full article
(This article belongs to the Special Issue Hydrogelated Matrices: Structural, Functional and Applicative Aspects)
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12 pages, 1437 KiB  
Article
Prevention of Dry Socket with Ozone Oil-Based Gel after Inferior Third Molar Extraction: A Double-Blind Split-Mouth Randomized Placebo-Controlled Clinical Trial
by Alberto Materni, Claudio Pasquale, Eugenio Longo, Massimo Frosecchi, Stefano Benedicenti, Matteo Bozzo and Andrea Amaroli
Gels 2023, 9(4), 289; https://doi.org/10.3390/gels9040289 - 1 Apr 2023
Cited by 6 | Viewed by 2860
Abstract
Tooth extraction is followed by a sequence of elaborate local changes affecting hard and soft tissues. Dry socket (DS) can occur as intense pain around and in the extraction site, with an incidence from 1–4% after generic tooth extraction to 45% for mandibular [...] Read more.
Tooth extraction is followed by a sequence of elaborate local changes affecting hard and soft tissues. Dry socket (DS) can occur as intense pain around and in the extraction site, with an incidence from 1–4% after generic tooth extraction to 45% for mandibular third molars. Ozone therapy has gained attention in the medical field because of its success in the treatment of various diseases, its biocompatible properties and its fewer side effects or discomfort than drugs. To investigate the preventive effect of the sunflower oil-based ozone gel Ozosan® (Sanipan srl, Clivio (VA), Italy) on DS, a double-blind split-mouth randomized placebo-controlled clinical trial was conducted according to the CONSORT guidelines. Ozosan® or the placebo gel were put in the socket, and the gels were washed off 2 min later. In total, 200 patients were included in our study. The patient population comprised 87 Caucasian males and 113 Caucasian females. The mean age of the included patients was 33.1 ± 12.4 years. Ozosan reduced the incidence of DS after inferior third molar extraction from 21.5% of the control to 2% (p < 0.001). Concerning the dry socket epidemiology, the incidence was not significantly correlated with gender, smoking or mesioangular, vertical or distoangular Winter’s classification. Post hoc power calculation showed a power of 99.8% for this data, with alpha = 0.001. Full article
(This article belongs to the Special Issue Hydrogelated Matrices: Structural, Functional and Applicative Aspects)
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