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Recent Advances of Mesoporous Materials and Their 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 (31 May 2022) | Viewed by 23549

Special Issue Editors


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Guest Editor
Departamento de Química Inorgánica, Cristalografía y Mineralogía (Unidad Asociada al ICP-CSIC), Facultad de Ciencias, Campus de Teatinos, Universidad de Málaga, 29071 Málaga, Spain
Interests: heterogeneous catalysis; mesoporous solids synthesis; acid–base catalysis; biomass valorization by means of catalytic processes
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Special Issue Information

Dear Colleagues,

Since the development of the M41S mesoporous silica family, a wide spectrum of possibilities has been opened for the synthesis of a myriad of mesoporous solids. These solids have found uses in many different fields of science, from catalysis or adsorption to biomedical applications. This fact is related to their properties, i.e., a high surface area, uniform pore size, large pore volume and ease of functionalizing its surface. One of most significant breakthroughs is related to carrying a determined drug to the target and releasing it on demand upon stimuli. The controlled and sustained release of drug molecules from the ordered mesoporous structure can reduce the total dose, which can cause side effects caused by overdosing of the drug and increase the efficiency of the drug action by increasing the local drug concentration.

The goal of this Special Issue is to provide the most recent advances on the synthesis, design, functionalization and uses of mesoporous solids in the different areas related to biomedical applications. Between these applications, this issue will highlight their uses as delivery vehicles for virtually any active molecule of choice, including small-molecular drugs, peptides, proteins, nucleic acids, as well as imaging agents and sensing molecules.

Dr. Ramón Moreno Tost
Dr. Juan Antonio Cecilia
Guest Editors

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Keywords

  • Mesoporous silica nanoparticles
  • Surface functionalization
  • Adsorption
  • Drug delivery
  • Biosafety
  • Selective targeting
  • Stimuli-responsive controlled release
  • Nanomedicine
  • Nanocomposites
  • Core-shell particles

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Published Papers (9 papers)

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Editorial

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3 pages, 216 KiB  
Editorial
Recent Advances in Mesoporous Materials and Their Biomedical Applications
by Juan Antonio Cecilia and Ramón Moreno-Tost
Int. J. Mol. Sci. 2022, 23(24), 15636; https://doi.org/10.3390/ijms232415636 - 9 Dec 2022
Cited by 4 | Viewed by 1130
Abstract
Since the beginning of civilization, porous materials have been used for medical purposes [...] Full article

Research

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10 pages, 2397 KiB  
Article
Facile Mesoporous Hollow Silica Synthesis for Formaldehyde Adsorption
by Misun Kang, Jong-tak Lee and Jae Young Bae
Int. J. Mol. Sci. 2023, 24(4), 4208; https://doi.org/10.3390/ijms24044208 - 20 Feb 2023
Cited by 14 | Viewed by 2191
Abstract
Formaldehyde emitted from household products is classified as a hazardous substance that can adversely affect human health. Recently, various studies related to adsorption materials for reducing formaldehyde have been widely reported. In this study, mesoporous and mesoporous hollow silicas with amine functional groups [...] Read more.
Formaldehyde emitted from household products is classified as a hazardous substance that can adversely affect human health. Recently, various studies related to adsorption materials for reducing formaldehyde have been widely reported. In this study, mesoporous and mesoporous hollow silicas with amine functional groups introduced were utilized as adsorption materials for formaldehyde. Formaldehyde adsorption characteristics of mesoporous and mesoporous hollow silicas having well-developed pores were compared based on their synthesis methods—with or without a calcination process. Mesoporous hollow silica synthesized through a non-calcination process had the best formaldehyde adsorption characteristics, followed by mesoporous hollow silica synthesized through a calcination process and mesoporous silica. This is because a hollow structure has better adsorption properties than mesoporous silica due to large internal pores. The specific surface area of mesoporous hollow silica synthesized without a calcination process was also higher than that synthesized with a calcination process, leading to a better adsorption performance. This research suggests a facile synthetic method of mesoporous hollow silica and confirms its noticeable potential as a support for the adsorption of harmful gases. Full article
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18 pages, 16552 KiB  
Article
Triantennary GalNAc-Functionalized Multi-Responsive Mesoporous Silica Nanoparticles for Drug Delivery Targeted at Asialoglycoprotein Receptor
by Rosemeyre Cordeiro, Ana Carvalho, Luísa Durães and Henrique Faneca
Int. J. Mol. Sci. 2022, 23(11), 6243; https://doi.org/10.3390/ijms23116243 - 2 Jun 2022
Cited by 9 | Viewed by 2749
Abstract
In recent years, mesoporous silica particles have been revealed as promising drug delivery systems combining high drug loading capacity, excellent biocompatibility, and easy and affordable synthetic and post-synthetic procedures. In fact, the straightforward functionalization approaches of these particles allow their conjugation with targeting [...] Read more.
In recent years, mesoporous silica particles have been revealed as promising drug delivery systems combining high drug loading capacity, excellent biocompatibility, and easy and affordable synthetic and post-synthetic procedures. In fact, the straightforward functionalization approaches of these particles allow their conjugation with targeting moieties in order to surpass one of the major challenges in drug administration, the absence of targeting ability of free drugs that reduces their therapeutic efficacy and causes undesired side effects. In this context, the main goal of this work was to develop a new targeted mesoporous silica nanoparticle formulation with the capability to specifically and efficiently deliver an anticancer drug to hepatocellular carcinoma (HCC) cells. To this purpose, and as proof of concept, we developed redox-responsive mesoporous silica nanoparticles functionalized with the targeting ligand triantennary N-acetylgalactosamine (GalNAc) cluster, which has high affinity to asialoglycoprotein receptors overexpressed in HCC cells, and loaded them with epirubicin, an anthracycline drug. The produced nanocarrier exhibits suitable physicochemical properties for drug delivery, high drug loading capacity, high biocompatibility, and targeting ability to HCC cells, revealing its biopharmaceutical potential as a targeted drug carrier for therapeutic applications in liver diseases. Full article
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18 pages, 9745 KiB  
Article
Identifying the Molecular Mechanisms and Types of Cell Death Induced by bio- and pyr-Silica Nanoparticles in Endothelial Cells
by Katarzyna Solarska-Ściuk, Kinga Adach, Mateusz Fijałkowski, Katarzyna Haczkiewicz-Leśniak, Michał Kulus, Mateusz Olbromski, Natalia Glatzel-Plucińska, Oskar Szelest and Dorota Bonarska-Kujawa
Int. J. Mol. Sci. 2022, 23(9), 5103; https://doi.org/10.3390/ijms23095103 - 4 May 2022
Cited by 5 | Viewed by 2330
Abstract
The term “nanosilica” refers to materials containing ultrafine particles. They have gained a rapid increase in popularity in a variety of applications and in numerous aspects of human life. Due to their unique physicochemical properties, SiO2 nanoparticles have attracted significant attention in [...] Read more.
The term “nanosilica” refers to materials containing ultrafine particles. They have gained a rapid increase in popularity in a variety of applications and in numerous aspects of human life. Due to their unique physicochemical properties, SiO2 nanoparticles have attracted significant attention in the field of biomedicine. This study aimed to elucidate the mechanism underlying the cellular response to stress which is induced by the exposure of cells to both biogenic and pyrogenic silica nanoparticles and which may lead to their death. Both TEM and fluorescence microscopy investigations confirmed molecular changes in cells after treatment with silica nanoparticles. The cytotoxic activity of the compounds and intracellular RNS were determined in relation to HMEC-1 cells using the fluorimetric method. Apoptosis was quantified by microscopic assessment and by flow cytometry. Furthermore, the impact of nanosilica on cell migration and cell cycle arrest were determined. The obtained results compared the biological effects of mesoporous silica nanoparticles extracted from Urtica dioica L. and pyrogenic material and indicated that both types of NPs have an impact on RNS production causing apoptosis, necrosis, and autophagy. Although mesoporous silica nanoparticles did not cause cell cycle arrest, at the concentration of 50 μg/mL and higher they could disturb redox balance and stimulate cell migration. Full article
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11 pages, 3183 KiB  
Article
The Role of the pH in the Impregnation of Spherical Mesoporous Silica Particles with L-Arginine Aqueous Solutions
by Sara Saber Younes Mohamed, Sonia Martinez, Mauro Banchero, Luigi Manna, Silvia Ronchetti and Barbara Onida
Int. J. Mol. Sci. 2021, 22(24), 13403; https://doi.org/10.3390/ijms222413403 - 14 Dec 2021
Cited by 1 | Viewed by 2927
Abstract
In the context of the development of carriers for amino acids delivery, Spherical Mesoporous Silica Particles (SMSP), characterized by particles size ranging from 0.15 µm to 0.80 µm and average pore diameter of 2.4 nm, were synthesised and loaded with L-arginine (ARG), a [...] Read more.
In the context of the development of carriers for amino acids delivery, Spherical Mesoporous Silica Particles (SMSP), characterized by particles size ranging from 0.15 µm to 0.80 µm and average pore diameter of 2.4 nm, were synthesised and loaded with L-arginine (ARG), a basic amino acid involved in several physiological processes. The loading was performed using water as a solvent through the wet impregnation method (with a final arginine content of 9.1% w/w). The material was characterized before and after impregnation by means of X-Ray Diffraction (XRD), nitrogen sorption analysis, Field Emission Scanning Electron Microscopy (FESEM) and Fourier Transform Infrared (FT-IR) spectroscopy. SMSP are shown to suffer degradation upon impregnation, which dramatically affects their porosity. To elucidate the role of the pH of the ARG impregnating solution (originally set at pH ≈ 11) on SMSP degradation, the loading was performed under different pH conditions (5 and 9) keeping constant the ARG concentration. The impregnation performed with acidic solution did not modify the carrier. All samples displayed ARG in amorphous form: zwitterionic species were present in SMSP impregnated at basic pH whereas positive protonated species in that impregnated at acidic pH. Full article
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22 pages, 5671 KiB  
Article
Influence of Injection Application on the Sol–Gel Phase Transition Conditions of Polysaccharide-Based Hydrogels
by Anna Rył and Piotr Owczarz
Int. J. Mol. Sci. 2021, 22(24), 13208; https://doi.org/10.3390/ijms222413208 - 8 Dec 2021
Cited by 7 | Viewed by 2609
Abstract
Polysaccharide matrices formed via thermoinduced sol–gel phase transition are promising systems used as drug carriers and minimally invasiveness scaffolds in tissue engineering. The strong shear field generated during injection may lead to changes in the conformation of polymer molecules and, consequently, affect the [...] Read more.
Polysaccharide matrices formed via thermoinduced sol–gel phase transition are promising systems used as drug carriers and minimally invasiveness scaffolds in tissue engineering. The strong shear field generated during injection may lead to changes in the conformation of polymer molecules and, consequently, affect the gelation conditions that have not been studied so far. Chitosan (CS) and hydroxypropyl cellulose (HPC) sols were injected through injection needles (14 G–25 G) or sheared directly in the rheometer measuring system. Then the sol–gel phase transition conditions were determined at 37 °C using rheometric, turbidimetric, and rheo-optical techniques. It was found that the use of low, respecting injection, shear rates accelerate the gelation, its increase extends the gelation time; applying the highest shear rates may significantly slow down (HPC) or accelerate gelation (CS) depending on thixotropic properties. From a practical point of view, the conducted research indicates that the use of thin needles without preliminary tests may lead to an extension of the gelation time and consequently the spilling of the polymeric carrier before gelation. Finally, an interpretation of the influence of an intensive shear field on the conformation of the molecules on a molecular scale was proposed. Full article
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24 pages, 3525 KiB  
Article
Protein Adsorption onto Modified Porous Silica by Single and Binary Human Serum Protein Solutions
by Diego R. Gondim, Juan A. Cecilia, Thaina N. B. Rodrigues, Enrique Vilarrasa-García, Enrique Rodríguez-Castellón, Diana C. S. Azevedo and Ivanildo J. Silva, Jr.
Int. J. Mol. Sci. 2021, 22(17), 9164; https://doi.org/10.3390/ijms22179164 - 25 Aug 2021
Cited by 5 | Viewed by 2304
Abstract
Typical porous silica (SBA-15) has been modified with pore expander agent (1,3,5-trimethylbenzene) and fluoride-species to diminish the length of the channels to obtain materials with different textural properties, varying the Si/Zr molar ratio between 20 and 5. These porous materials were characterized by [...] Read more.
Typical porous silica (SBA-15) has been modified with pore expander agent (1,3,5-trimethylbenzene) and fluoride-species to diminish the length of the channels to obtain materials with different textural properties, varying the Si/Zr molar ratio between 20 and 5. These porous materials were characterized by X-ray Diffraction (XRD), N2 adsorption/desorption isotherms at −196 °C and X-ray Photoelectron Spectroscopy (XPS), obtaining adsorbent with a surface area between 420–337 m2 g−1 and an average pore diameter with a maximum between 20–25 nm. These materials were studied in the adsorption of human blood serum proteins (human serum albumin—HSA and immunoglobulin G—IgG). Generally, the incorporation of small proportions was favorable for proteins adsorption. The adsorption data revealed that the maximum adsorption capacity was reached close to the pI. The batch purification experiments in binary human serum solutions showed that Si sample has considerable adsorption for IgG while HSA adsorption is relatively low, so it is possible its separation. Full article
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13 pages, 2871 KiB  
Article
Kidney-Protector Lipidic Cilastatin Derivatives as Structure-Directing Agents for the Synthesis of Mesoporous Silica Nanoparticles for Drug Delivery
by Samuel Martinez-Erro, Francisco Navas, Eva Romaní-Cubells, Paloma Fernández-García, Victoria Morales, Raul Sanz and Rafael A. García-Muñoz
Int. J. Mol. Sci. 2021, 22(15), 7968; https://doi.org/10.3390/ijms22157968 - 26 Jul 2021
Cited by 7 | Viewed by 2456
Abstract
Mesoporous silica nanomaterials have emerged as promising vehicles in controlled drug delivery systems due to their ability to selectively transport, protect, and release pharmaceuticals in a controlled and sustained manner. One drawback of these drug delivery systems is their preparation procedure that usually [...] Read more.
Mesoporous silica nanomaterials have emerged as promising vehicles in controlled drug delivery systems due to their ability to selectively transport, protect, and release pharmaceuticals in a controlled and sustained manner. One drawback of these drug delivery systems is their preparation procedure that usually requires several steps including the removal of the structure-directing agent (surfactant) and the later loading of the drug into the porous structure. Herein, we describe the preparation of mesoporous silica nanoparticles, as drug delivery systems from structure-directing agents based on the kidney-protector drug cilastatin in a simple, fast, and one-step process. The concept of drug-structure-directing agent (DSDA) allows the use of lipidic derivatives of cilastatin to direct the successful formation of mesoporous silica nanoparticles (MSNs). The inherent pharmacological activity of the surfactant DSDA cilastatin-based template permits that the MSNs can be directly employed as drug delivery nanocarriers, without the need of extra steps. MSNs thus synthesized have shown good sphericity and remarkable textural properties. The size of the nanoparticles can be adjusted by simply selecting the stirring speed, time, and aging temperature during the synthesis procedure. Moreover, the release experiments performed on these materials afforded a slow and sustained drug release over several days, which illustrates the MSNs potential utility as drug delivery system for the cilastatin cargo kidney protector. While most nanotechnology strategies focused on combating the different illnesses this methodology emphasizes on reducing the kidney toxicity associated to cancer chemotherapy. Full article
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Review

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43 pages, 3784 KiB  
Review
The Role of Copper in the Hydrogenation of Furfural and Levulinic Acid
by Cristina García-Sancho, Josefa María Mérida-Robles, Juan Antonio Cecilia-Buenestado, Ramón Moreno-Tost and Pedro Jesús Maireles-Torres
Int. J. Mol. Sci. 2023, 24(3), 2443; https://doi.org/10.3390/ijms24032443 - 26 Jan 2023
Cited by 11 | Viewed by 3547
Abstract
Currently, there is a great interest in the development of sustainable and green technologies for production of biofuels and chemicals. In this sense, much attention is being paid to lignocellulosic biomass as feedstock, as alternative to fossil-based resources, inasmuch as its fractions can [...] Read more.
Currently, there is a great interest in the development of sustainable and green technologies for production of biofuels and chemicals. In this sense, much attention is being paid to lignocellulosic biomass as feedstock, as alternative to fossil-based resources, inasmuch as its fractions can be transformed into value-added chemicals. Two important platform molecules derived from lignocellulosic sugars are furfural and levulinic acid, which can be transformed into a large spectrum of chemicals, by hydrogenation, oxidation, or condensation, with applications as solvents, agrochemicals, fragrances, pharmaceuticals, among others. However, in many cases, noble metal-based catalysts, scarce and expensive, are used. Therefore, an important effort is performed to search the most abundant, readily available, and cheap transition-metal-based catalysts. Among these, copper-based catalysts have been proposed, and the present review deals with the hydrogenation of furfural and levulinic acid, with Cu-based catalysts, into several relevant chemicals: furfuryl alcohol, 2-methylfuran, and cyclopentanone from FUR, and γ-valerolactone and 2-methyltetrahydrofuran from LA. Special emphasis has been placed on catalytic processes used (gas- and liquid-phase, catalytic transfer hydrogenation), under heterogeneous catalysis. Moreover, the effect of addition of other metal to Cu-based catalysts has been considered, as well as the issue related to catalyst stability in reusing studies. Full article
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