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Biomaterials Synthesized via Sol–Gel Methods

A special issue of Materials (ISSN 1996-1944).

Deadline for manuscript submissions: closed (30 September 2021) | Viewed by 25366

Special Issue Editor


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Guest Editor
Department of Engineering, University of Campania “Luigi Vanvitelli”, Via Roma 29, I-81031 Aversa, Italy
Interests: sol-gel technology; biomaterials; bioglass; organic-inorganic hybrid materials; drug delivery; thin films
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Special Issue Information

Dear Colleagues,

The requirement of improving the life quality of people affected by diseases that need replacements of tissues or body parts has encouraged the development of new materials with high performance in terms of tolerability and integration capability. These promising so-called "Biomaterials" are able to interact with human tissue and body fluids to treat, improve, or replace anatomical elements of the human body, without adverse reactions in the host organism. They can be applied to permanent structures such as implants and artificial organs or devices that stay in contact with the human body for a limited time such as sutures or scaffolds. Despite advances in the biomaterials field, today a good combination between properties (mechanical, chemical, and tribological) and biocompatibility of the materials has not been yet achieved. This is the cause of the early failure of the implants, which entails the need for the subsequent replacement of the prosthetic devices, especially in young patients.

An ideal method to prepare biomaterials is the sol–gel technique. It is a versatile synthesis process used to produce ceramics and/or glasses materials at low temperatures.

The process starts when water is added to a solution of metal alkoxyde precursors in alcohol. The hydrolysis of metal alkoxide precursor and the polycondensation of the formed oligomers cause the transition of the system from a mostly colloidal liquid (sol) into a solid (gel). By drying the obtained wet gel, it is possible to prepare xerogels (by exposure to low temperatures) or aerogels (by solvent extraction under supercritical conditions) or dense ceramic and glass by means of a further heat treatment at higher temperatures. The sol–gel method has many advantages, such as the purity of products and the possibility of controlling the chemical composition, the microstructure and, thus, the properties of the obtained materials through the modulation of the parameters of the sol–gel process, such as the molar ratios of the reagents, pH, inhibitor/catalyst addition, and heat treatment. Moreover, sol–gel chemistry and the low processing temperature used allow for embedding in inorganic glassy materials of various thermolabile molecules (e.g., polymers, drugs, biomolecules, etc.) during the formation of the glassy matrix, via the dissolution of those molecules in a liquid sol–gel system, producing organic/inorganic hybrids.

Assoc. Prof. Michelina Catauro
Guest Editor

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Keywords

  • biomaterials
  • drug delivery
  • sol-gel method
  • hybrid materials
  • bioactivity
  • biocompatibility
  • cell viability

Published Papers (6 papers)

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Research

13 pages, 3087 KiB  
Article
Surface Interactions between Ketoprofen and Silica-Based Biomaterials as Drug Delivery System Synthesized via Sol–Gel: A Molecular Dynamics Study
by Giuseppina Raffaini and Michelina Catauro
Materials 2022, 15(8), 2759; https://doi.org/10.3390/ma15082759 - 08 Apr 2022
Cited by 10 | Viewed by 2516
Abstract
Biomaterial-based drug delivery systems for a controlled drug release are drawing increasing attention thanks to their possible pharmaceutical and biomedical applications. It is important to control the local administration of drugs, especially when the drug exhibits problems diffusing across biological barriers. Thus, in [...] Read more.
Biomaterial-based drug delivery systems for a controlled drug release are drawing increasing attention thanks to their possible pharmaceutical and biomedical applications. It is important to control the local administration of drugs, especially when the drug exhibits problems diffusing across biological barriers. Thus, in an appropriate concentration, it would be released in situ, reducing side effects due to interactions with the biological environment after implantation. A theoretical study based on Molecular Mechanics and Molecular Dynamics methods is performed to investigate possible surface interactions between the amorphous SiO2 surface and the ketoprofen molecules, an anti-inflammatory drug, considering the role of drug concentration. These theoretical results are compared with experimental data obtained by analyzing, through Fourier transform infrared spectroscopy (FT-IR), the interaction between the SiO2 amorphous surface and two percentages of the ketoprofen drug entrapped in a silica matrix obtained via the sol–gel method and dried materials. The loaded drug in these amorphous bioactive material forms hydrogen bonds with the silica surface, as found in this theoretical study. The surface interactions are essential to have a new generation of biomaterials not only important for biocompatibility, with specific structural and functional properties, but also able to incorporate anti-inflammatory agents for release into the human body. Full article
(This article belongs to the Special Issue Biomaterials Synthesized via Sol–Gel Methods)
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17 pages, 4769 KiB  
Article
Comparison of Mechanical and Barrier Properties of Al2O3/TiO2/ZrO2 Layers in Oxide–Hydroxyapatite Sandwich Composite Coatings Deposited by Sol–Gel Method on Ti6Al7Nb Alloy
by Bożena Pietrzyk, Daniel Kucharski, Łukasz Kołodziejczyk, Sebastian Miszczak and Mateusz Fijalkowski
Materials 2020, 13(3), 502; https://doi.org/10.3390/ma13030502 - 21 Jan 2020
Cited by 7 | Viewed by 3266
Abstract
In this study, coatings of different oxides (TiO2, Al2O3, ZrO2) and hydroxyapatite (HAp) as well as sandwich composite hydroxyapatite with an oxides sublayer (oxide+HAp) were deposited on Ti6Al7Nb alloy using the sol–gel dip-coating method. The [...] Read more.
In this study, coatings of different oxides (TiO2, Al2O3, ZrO2) and hydroxyapatite (HAp) as well as sandwich composite hydroxyapatite with an oxides sublayer (oxide+HAp) were deposited on Ti6Al7Nb alloy using the sol–gel dip-coating method. The coatings were characterized in terms of morphology (optical microscope), surface topography (AFM), thickness (ellipsometry), and crystal structure (XRD/GIXRD). The mechanical properties of the coatings—hardness, Young’s modulus, and adhesion to the substrate—were examined using nanoindentation and scratch tests. The barrier properties of the coatings against the migration of aluminum ions were examined by measuring their concentration after soaking in Hank’s balanced salt solution (HBSS) with the use of optical emission spectrometry of inductively coupled plasma (ICPOES). It was found that all the oxide and HAp coatings reduced the permeation of Al ions from the Ti6Al7Nb alloy substrate. The best features revealed an Al2O3 layer that had excellent barrier properties and the best adhesion to the substrate. Al2O3 as a sublayer significantly improved the properties of the sandwich composite HAp coating. Full article
(This article belongs to the Special Issue Biomaterials Synthesized via Sol–Gel Methods)
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12 pages, 2987 KiB  
Article
New SiO2/Caffeic Acid Hybrid Materials: Synthesis, Spectroscopic Characterization, and Bioactivity
by Michelina Catauro, Federico Barrino, Giovanni Dal Poggetto, Giuseppina Crescente, Simona Piccolella and Severina Pacifico
Materials 2020, 13(2), 394; https://doi.org/10.3390/ma13020394 - 15 Jan 2020
Cited by 44 | Viewed by 3281
Abstract
The sol–gel route represents a valuable technique to obtain functional materials, in which organic and inorganic members are closely connected. Herein, four hybrid materials, containing caffeic acid entrapped in a silica matrix at 5, 10, 15, and 20 wt.%, were synthesized and characterized [...] Read more.
The sol–gel route represents a valuable technique to obtain functional materials, in which organic and inorganic members are closely connected. Herein, four hybrid materials, containing caffeic acid entrapped in a silica matrix at 5, 10, 15, and 20 wt.%, were synthesized and characterized through Fourier-Transform Infrared (FT-IR) and Ultraviolet-Visible (UV–Vis) spectroscopy. FT-IR analysis was also performed to evaluate the ability to induce the hydroxyapatite nucleation. Despite some structural changes occurring on the phenol molecular skeleton, hybrid materials showed scavenging properties vs. 2,2-diphenyl-1-picrylhydrazyl (DPPH) radical and 2,2′-azinobis-(3-ethylbenzothiazolin-6-sulfonic acid) radical cation (ABTS•+), which was dependent on the tested dose and on the caffeic acid wt.%. The SiO2/caffeic acid materials are proposed as valuable antibacterial agents against Escherichia coli and Enterococcus faecalis. Full article
(This article belongs to the Special Issue Biomaterials Synthesized via Sol–Gel Methods)
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12 pages, 2904 KiB  
Article
Sol–Gel Synthesis of Silica-Based Materials with Different Percentages of PEG or PCL and High Chlorogenic Acid Content
by Elisabetta Tranquillo, Federico Barrino, Giovanni Dal Poggetto and Ignazio Blanco
Materials 2019, 12(1), 155; https://doi.org/10.3390/ma12010155 - 06 Jan 2019
Cited by 51 | Viewed by 5568
Abstract
Implanted biomedical devices can induce adverse responses in the human body, which can cause failure of the implant—referred to as implant failure. Early implant failure is induced numerous factors, most importantly, infection and inflammation. Natural products are, today, one of the main sources [...] Read more.
Implanted biomedical devices can induce adverse responses in the human body, which can cause failure of the implant—referred to as implant failure. Early implant failure is induced numerous factors, most importantly, infection and inflammation. Natural products are, today, one of the main sources of new drug molecules due to the development of pathogenic bacterial strains that possess resistance to more antibiotics used currently in various diseases. The aim of this work is the sol–gel synthesis of antibacterial biomedical implants. In the silica matrix, different percentages (6, 12, 24, 50 wt %) of polyethylene glycol (PEG) or poly(ε-caprolactone) (PCL) were embedded. Subsequently, the ethanol solutions with high amounts of chlorogenic acid (CGA 20 wt %) were slowly added to SiO2/PEG and SiO2/PCL sol. The interactions among different organic and inorganic phases in the hybrid materials was studied by Fourier transform infrared (FTIR) spectroscopy. Furthermore, the materials were soaked in simulated body fluid (SBF) for 21 days and the formation of a hydroxyapatite layer on their surface was evaluated by FTIR and XRD analysis. Finally, Escherichia coli and Pseudomonas aeruginosa were incubated with several hybrids, and the diameter of zone of inhibition was observed to assessment the potential antibacterial properties of the hybrids. Full article
(This article belongs to the Special Issue Biomaterials Synthesized via Sol–Gel Methods)
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11 pages, 3475 KiB  
Article
Chlorogenic Acid Entrapped in Hybrid Materials with High PEG Content: A Strategy to Obtain Antioxidant Functionalized Biomaterials?
by Michelina Catauro, Federico Barrino, Giovanni Dal Poggetto, Giuseppina Crescente, Simona Piccolella and Severina Pacifico
Materials 2019, 12(1), 148; https://doi.org/10.3390/ma12010148 - 04 Jan 2019
Cited by 29 | Viewed by 2976
Abstract
The formation of pro-oxidant species after implantation of biomaterials could be responsible for the failure of the implant itself, because of oxidative stress-induced damage. In this work, the SiO2/polyethylene glycol (PEG)/chlorogenic acid (CGA) hybrids synthesized by the sol–gel method with 50 [...] Read more.
The formation of pro-oxidant species after implantation of biomaterials could be responsible for the failure of the implant itself, because of oxidative stress-induced damage. In this work, the SiO2/polyethylene glycol (PEG)/chlorogenic acid (CGA) hybrids synthesized by the sol–gel method with 50 wt% of the polymer and different amounts of CGA (5, 10, 15 and 20 wt%) were studied. The hybrids soaked in simulated body fluid (SBF) showed the formation of hydroxyapatite layers on their surface, suggesting that the hybrids are bioactive. Their radical scavenging capacity towards DPPH· and ABTS·+ (2,2′-Azino-bis(3-ethylbenzthiazoline-6-sulfonic acid), evaluated at three different doses (0.5, 1 and 2 mg), showed probe- and dose-dependent behavior. In addition, the antioxidant properties of CGA were not affected by the presence of high amounts of the polymer. The in vitro biocompatibility in three cell lines (NIH 3T3, HaCaT and SH-SY5Y) was assessed by using the 3-(4,5-dimethyl-2-thiazolyl)-2,5-diphenyl-2H-tetrazolium bromide (MTT) assay. Apart from SH-SY5Y, the cell viability—expressed as mitochondrial redox activity percentage of cells directly exposed to powders—and morphology was not affected, suggesting that the hybrids have the ability to interfere and act selectively against tumor cells. The antibacterial properties of the different materials against Escherichia coli and Enterococcus faecalis were affected by different amounts of the natural antioxidant component. Full article
(This article belongs to the Special Issue Biomaterials Synthesized via Sol–Gel Methods)
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11 pages, 2556 KiB  
Article
Influence of the Heat Treatment on the Particles Size and on the Crystalline Phase of TiO2 Synthesized by the Sol-Gel Method
by Michelina Catauro, Elisabetta Tranquillo, Giovanni Dal Poggetto, Mauro Pasquali, Alessandro Dell’Era and Stefano Vecchio Ciprioti
Materials 2018, 11(12), 2364; https://doi.org/10.3390/ma11122364 - 24 Nov 2018
Cited by 89 | Viewed by 6844
Abstract
Titanium biomaterials’ response has been recognized to be affected by particles size, crystal structure, and surface properties. Chemical and structural properties of these nanoparticle materials are important, but their size is the key aspect. The aim of this study is the synthesis of [...] Read more.
Titanium biomaterials’ response has been recognized to be affected by particles size, crystal structure, and surface properties. Chemical and structural properties of these nanoparticle materials are important, but their size is the key aspect. The aim of this study is the synthesis of TiO2 nanoparticles by the sol-gel method, which is an ideal technique to prepare nanomaterials at low temperature. The heat treatment can affect the structure of the final product and consequently its biological properties. For this reason, the chemical structure of the TiO2 nanoparticles synthesized was investigated after each heat treatment, in order to evaluate the presence of different phases formed among the nanoparticles. FTIR spectroscopy and XRD have been used to evaluate the different structures. The results of these analyses suggest that an increase of the calcination temperature induces the formation of mixed-crystalline-phases with different content of anatase and rutile phases. The results obtained by SEM measurements suggest that an increase in the particles size accompanied by a noticeable aggregation of TiO2 nanoparticles is due to high temperatures achieved during the thermal treatments and confirmed the presence of different content of the two crystalline phases of titanium dioxide. Full article
(This article belongs to the Special Issue Biomaterials Synthesized via Sol–Gel Methods)
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