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Mesoporous Materials: From Synthesis to Applications

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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 (28 December 2018) | Viewed by 55850

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Special Issue Editors

Dr. Juan Antonio Cecilia

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Departamento de Química Inorgánica, Cristalografía y Mineralogía, Universidad de Málaga, 29071 Málaga, Spain
Interests: adsorption; biomass valorization; heterogeneous catalysis; high-added value products
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Dr. Ramón Moreno Tost

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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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Dr. María Retuerto Millán

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Instituto de Catálisis y Petroleoquímica, Madrid, Spain
Interests: synthesis of materials; characterization of materials

Special Issue Information

Dear Colleagues:

Porous materials are structures with a high specific surface area, narrow pore size distribution and tuneable pore size distribution. These materials have emerged as interesting frameworks for the scientific community due their high potential in various areas, including adsorption, separation, sensing, and catalysis. The rational design of these porous structures has led to innovative materials with a wide range of structures, such as hexagonal, lamellar, rod-like or cubic in silicates, aluminosilicates, metal oxides or carbons. The obtained materials display a wide variety of funcionalities that currently makes this field one of the most developed in materials science. However, many advances in the field are recently diversifying this exciting area of work to promising applications in drug delivery, tumoral therapy, biomedicine, desing of tuneable catalysts, etc.

This Special Issue is aimed to provide a range of original contributions detailing the synthesis, design, characterization and applications in different areas of porous materials (e.g., catalysis, separation, sensing, adsorption, drug delivery, etc).

Dr. Juan A. Cecilia
Dr. Ramón Moreno Tost
Dr. María Retuerto Millán
Guest Editors

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Keywords

Mesoporous materials
Metal organic frameworks (MOFs)
Metal oxides
Zeolites
Carbon
Adsorption
Catalysis
Catalytic support
Biomolecules
Drug delivery

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Published Papers (11 papers)

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Editorial

Jump to: Research

4 pages, 195 KiB

Open AccessEditorial

Mesoporous Materials: From Synthesis to Applications

by Juan Antonio Cecilia, Ramón Moreno Tost and María Retuerto Millán

Int. J. Mol. Sci. 2019, 20(13), 3213; https://doi.org/10.3390/ijms20133213 - 30 Jun 2019

Cited by 28 | Viewed by 4319

Abstract

Mesoporous silica are inorganic materials, which are formed by the condensation of sodium silicate or silicon alkoxides around an ordered surfactant used as template [...] Full article

(This article belongs to the Special Issue Mesoporous Materials: From Synthesis to Applications)

Research

Jump to: Editorial

15 pages, 2674 KiB

Open AccessArticle

Hydrogel-Encapsulated Mesoporous Silica-Coated Gold Nanoshells for Smart Drug Delivery

by Bo Sang Kim, Yi-Ting Chen, Pannaree Srinoi, Maria D. Marquez and T. Randall Lee

Int. J. Mol. Sci. 2019, 20(14), 3422; https://doi.org/10.3390/ijms20143422 - 12 Jul 2019

Cited by 13 | Viewed by 4259

Abstract

A “smart” core@shell composite nanoparticle (NP) having dual-response mechanisms (i.e., temperature and light) was synthesized, and its efficacy in the loading and release of small molecules was explored. These core@shell NPs are composed of an optically active gold nanoshell (GNS) core and a mesoporous (m-) silica layer (m-SiO₂). The GNS@m-SiO₂ nanoparticles are further encapsulated within a thermo-responsive poly(N-isopropylacrylamide-co-acrylic acid) hydrogel (PNIPAM-co-AA). The multi-responsive composite NPs were designed to create thermally and optically modulated drug-delivery vehicles with a m-SiO₂ layer providing additional non-collapsible space for drug storage. The influence of the m-SiO₂ layer on the efficacy of loading and release of methylene blue, which serves as a model for a small-molecule therapeutic drug, was evaluated. The “smart” core@shell composite NPs having a m-SiO₂ layer demonstrated an improved capacity to load and release small molecules compared to the corresponding NPs with no m-SiO₂ shell. Additionally, an efficient response by the composite NPs was successfully induced by the thermal energy generated from the gold nanoshell core upon exposure to near infrared (NIR) stimulation. Full article

(This article belongs to the Special Issue Mesoporous Materials: From Synthesis to Applications)

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19 pages, 4945 KiB

Open AccessArticle

Comparison of Polydopamine-Coated Mesoporous Silica Nanorods and Spheres for the Delivery of Hydrophilic and Hydrophobic Anticancer Drugs

by Anna-Karin Pada, Diti Desai, Kaiyao Sun, Narayana Prakirth Govardhanam, Kid Törnquist, Jixi Zhang and Jessica M. Rosenholm

Int. J. Mol. Sci. 2019, 20(14), 3408; https://doi.org/10.3390/ijms20143408 - 11 Jul 2019

Cited by 34 | Viewed by 5298

Abstract

Mesoporous silica nanoparticles (MSNs) have been widely studied as drug delivery systems in nanomedicine. Surface coating of MSNs have enabled them to perform efficiently in terms of bioavailability, biocompatibility, therapeutic efficacy and targeting capability. Recent studies have suggested the use of polydopamine (PDA) as a facilitative coating for MSNs that provides sustained and pH-responsive drug release, owing to the adhesive “molecular-glue” function of PDA. This further endows these hybrid MSN@PDA particles with the ability to carry large amounts of hydrophilic drugs. In this study, we expand the feasibility of this platform in terms of exploring its ability to also deliver hydrophobic drugs, as well as investigate the effect of particle shape on intracellular delivery of both a hydrophilic and hydrophobic anticancer drug. MSN@PDA loaded with doxorubicin (hydrophilic) and fingolimod (hydrophobic) was studied via a systematic in vitro approach (cellular internalization, intracellular drug distribution and cytotoxicity). To promote the cellular uptake of the MSN@PDA particles, they were further coated with a polyethylene imine (PEI)-polyethylene glycol (PEG) copolymer. Drug-loaded, copolymer-coated MSN@PDA showed effective cellular uptake, intracellular release and an amplified cytotoxic effect with both doxorubicin and fingolimod. Additionally, rods exhibited delayed intracellular drug release and superior intracellular uptake compared to spheres. Hence, the study provides an example of how the choice and design of drug delivery systems can be tuned by the need for performance, and confirms the PDA coating of MSNs as a useful drug delivery platform beyond hydrophilic drugs. Full article

(This article belongs to the Special Issue Mesoporous Materials: From Synthesis to Applications)

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13 pages, 3348 KiB

Open AccessArticle

Microwave-Synthesized Platinum-Embedded Mesoporous Silica Nanoparticles as Dual-Modality Contrast Agents: Computed Tomography and Optical Imaging

by Chia-Hui Chu, Shih-Hsun Cheng, Nai-Tzu Chen, Wei-Neng Liao and Leu-Wei Lo

Int. J. Mol. Sci. 2019, 20(7), 1560; https://doi.org/10.3390/ijms20071560 - 28 Mar 2019

Cited by 24 | Viewed by 3994

Abstract

Nanoparticle-based imaging contrast agents have drawn tremendous attention especially in multi-modality imaging. In this study, we developed mesoporous silica nanoparticles (MSNs) for use as dual-modality contrast agents for computed tomography (CT) and near-infrared (NIR) optical imaging (OI). A microwave synthesis for preparing naked platinum nanoparticles (nPtNPs) on MSNs (MSNs-Pt) was developed and characterized with physicochemical analysis and imaging systems. The high density of nPtNPs on the surface of the MSNs could greatly enhance the CT contrast. Inductively coupled plasma mass spectrometry (ICP-MS) revealed the MSNs-Pt compositions to be ~14% Pt by weight and TEM revealed an average particle diameter of ~50 nm and covered with ~3 nm diameter nPtNPs. To enhance the OI contrast, the NIR fluorescent dye Dy800 was conjugated to the MSNs-Pt nanochannels. The fluorescence spectra of MSNs-Pt-Dy800 were very similar to unconjugated Dy800. The CT imaging demonstrated that even modest degrees of Pt labeling could result in substantial X-ray attenuation. In vivo imaging of breast tumor-bearing mice treated with PEGylated MSNs-Pt-Dy800 (PEG-MSNs-Pt-Dy800) showed significantly improved contrasts in both fluorescence and CT imaging and the signal intensity within the tumor retained for 24 h post-injection. Full article

(This article belongs to the Special Issue Mesoporous Materials: From Synthesis to Applications)

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13 pages, 3582 KiB

Open AccessArticle

Sulfonate-Functionalized Mesoporous Silica Nanoparticles as Carriers for Controlled Herbicide Diquat Dibromide Release through Electrostatic Interaction

by Yongpan Shan, Lidong Cao, Chunli Xu, Pengyue Zhao, Chong Cao, Fengmin Li, Bo Xu and Qiliang Huang

Int. J. Mol. Sci. 2019, 20(6), 1330; https://doi.org/10.3390/ijms20061330 - 16 Mar 2019

Cited by 44 | Viewed by 5718

Abstract

Environmental stimuli-responsive pesticide release is desirable for enhanced efficiency and reduced side effects. In most cases, the loading and release of pesticides mainly depends on hydrophobic interactions and hydrogen bonding. Electrostatic interaction is less investigated as a weapon for achieving high loading content and controlled pesticide release. In this work, negative-charge decorated mesoporous silica nanoparticles (MSNs) were facilely fabricated by introducing sulfonate groups onto MSNs through a post-grafting method. Sulfonate-functionalized MSNs (MSN-SO₃) were synthesized by conversion of epoxy group into sulfonate group using a bisulfite ion as a ring opening reagent. Diquat dibromide (DQ), one of the globally used quaternary ammonium herbicides, was efficiently loaded into these negatively charged MSN-SO₃ nanoparticles. The loading content was increased to 12.73% compared to those using bare MSNs as carriers (5.31%). The release of DQ from DQ@MSN-SO₃ nanoparticles was pH and ionic strength responsive, which was chiefly governed by the electrostatic interactions. Moreover, DQ@MSN-SO₃ nanoparticles exhibited good herbicidal activity for the control of Datura stramonium L., and the bioactivity was affected by the ionic strength of the release medium. The strategy of cargo loading and release dependent on the electrostatic interactions could be generally used for charge-carrying pesticides using carriers possessing opposite charges to mitigate the potential negative impacts on the environment. Full article

(This article belongs to the Special Issue Mesoporous Materials: From Synthesis to Applications)

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22 pages, 7712 KiB

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Influence of Structure-modifying Agents in the Synthesis of Zr-doped SBA-15 Silica and Their Use as Catalysts in the Furfural Hydrogenation to Obtain High Value-added Products through the Meerwein-Ponndorf-Verley Reduction

by Raquel López-Asensio, Carmen Pilar Jiménez Gómez, Cristina García Sancho, Ramón Moreno-Tost, Juan Antonio Cecilia and Pedro Maireles-Torres

Int. J. Mol. Sci. 2019, 20(4), 828; https://doi.org/10.3390/ijms20040828 - 14 Feb 2019

Cited by 28 | Viewed by 4205

Abstract

Zr-doped mesoporous silicas with different textural parameters have been synthesized in the presence of structure-modifying agents, and then characterized by X-ray diffraction (XRD), transmission electron microscopy (TEM), N₂ adsorption-desorption at −196 °C, NH₃ thermoprogrammed desorption (NH₃–TPD), CO₂ thermoprogrammed desorption (CO₂–TPD), and X-ray photoelectron spectroscopy (XPS). These porous materials were evaluated in the furfural hydrogenation through the Meerwein-Ponndorf-Verley (MPV) reaction. The catalytic results indicate that the catalyst synthesized under hydrothermal conditions and adding a pore expander agent is more active and selective to furfuryl alcohol. However, the Zr-doped porous silica catalysts that were synthesized at room temperature, which possess narrow pore sizes, tend to form i-propyl furfuryl and difurfuryl ethers, coming from etherification between furfuryl alcohol (FOL) and isopropanol molecules (used as H-donor) by a S_N2 mechanism. Full article

(This article belongs to the Special Issue Mesoporous Materials: From Synthesis to Applications)

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13 pages, 5377 KiB

Open AccessArticle

Molecular Simulation of Naphthalene, Phenanthrene, and Pyrene Adsorption on MCM-41

by Xiong Yang, Chuanzhao Zhang, Lijun Jiang, Ziyi Li, Yingshu Liu, Haoyu Wang, Yi Xing and Ralph T. Yang

Int. J. Mol. Sci. 2019, 20(3), 665; https://doi.org/10.3390/ijms20030665 - 3 Feb 2019

Cited by 15 | Viewed by 4578

Abstract

The adsorption of three typical polycyclic aromatic hydrocarbons (PAHs), naphthalene, phenanthrene, and pyrene with different ring numbers, on a common mesoporous material (MCM-41) was simulated based on a well-validated model. The adsorption equilibriums (isotherms), states (angle distributions and density profiles), and interactions (radial distribution functions) of three PAHs within the mesopores were studied in detail. The results show that the simulated isotherms agreed with previous experimental results. Each of the PAHs with flat molecules showed an adsorption configuration that was parallel to the surface of the pore, in the following order according to the degree of arrangement: pyrene (Pyr) > phenanthrene (Phe) > naphthalene (Nap). In terms of the interaction forces, there were no hydrogen bonds or other strong polar forces between the PAHs and MCM-41, and the O–H bond on the adsorbent surface had a unique angle in relation to the PAH molecular plane. The polarities of different H atoms on the PAHs were roughly the same, while those of the C atoms on the PAHs decreased from the molecular centers to the edges. The increasing area of the π-electron plane on the PAHs with the increasing ring number could lead to stronger adsorption interactions, and thus a shorter distance between the adsorbate and the adsorbent. Full article

(This article belongs to the Special Issue Mesoporous Materials: From Synthesis to Applications)

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21 pages, 2202 KiB

Open AccessArticle

Steam Reforming of Model Bio-Oil Aqueous Fraction Using Ni-(Cu, Co, Cr)/SBA-15 Catalysts

by José A. Calles, Alicia Carrero, Arturo J. Vizcaíno, Lourdes García-Moreno and Pedro J. Megía

Int. J. Mol. Sci. 2019, 20(3), 512; https://doi.org/10.3390/ijms20030512 - 25 Jan 2019

Cited by 44 | Viewed by 5244

Abstract

Hydrogen obtained from biomass derivatives is considered a promising alternative to fossil fuels. The aim of this work is to test the viability of Ni-M/SBA-15 (M: Co, Cu, Cr) catalysts for the hydrogen production from bio-oil aqueous fraction reforming. Tests were performed in a fixed-bed reactor at 600 °C and atmospheric pressure. Firstly, the steam reforming (SR) of acetic acid, hydroxyacetone, furfural and phenol, as representative constituents of the bio-oil aqueous fraction, was carried out. Lower reactivity with increasing carbon number and decreasing steam-to-carbon ratio was observed. Coking rate during SR is a consequence of carbon number and aromaticity of the reactant, as well as the steam-to-carbon ratio. However, deactivation also depends on the graphitization degree of carbon filaments, higher in the case of coke formed from phenol. Then, the performance of the Ni-M/SBA-15 catalysts was studied in the reforming of a bio-oil aqueous fraction surrogate containing the four model compounds. Ni-Co/SBA-15 and Ni-Cr/SBA-15 samples were the most active because Co also catalyze the steam reforming reactions and Cr promotes the formation of very small Ni crystallites accounting for high conversion and the low coke deposition (~8 times lower than Ni/SBA-15) in the form of poorly condensed carbon filaments. Full article

(This article belongs to the Special Issue Mesoporous Materials: From Synthesis to Applications)

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17 pages, 3375 KiB

Open AccessArticle

Electrochemical Detection of Dopamine at a Gold Electrode Modified with a Polypyrrole–Mesoporous Silica Molecular Sieves (MCM-48) Film

by Izabela Zablocka, Monika Wysocka-Zolopa and Krzysztof Winkler

Int. J. Mol. Sci. 2019, 20(1), 111; https://doi.org/10.3390/ijms20010111 - 29 Dec 2018

Cited by 40 | Viewed by 6562

Abstract

A gold electrode modified with a polypyrrole–mesoporous silica molecular sieves (polypyrrole—MCM-48) nanostructure film was used for the electrochemical determination of small concentrations of dopamine (DA) by cyclic voltammetry and square-wave voltammetry techniques. This electrode showed good electrocatalytic activity for the oxidation of dopamine. The oxidation potential of dopamine was decreased significantly compared with that obtained at the bare gold electrode. The observed linear range for the determination of the dopamine concentration, without interferents through cyclic voltammetry measurements, was from 10 μM to 1.2 mM (R² = 0.9989) for the gold electrode modified with the polypyrrole—MCM-48 nanostructure, with a detection limit of 2.5 μM. In the case of square-wave voltammetry, the linear range was 2–250 μM, with a correlation coefficient of 0.9996, and the detection limit was estimated to be 0.7 μM. The effects of interferents, such as ascorbic acid (AA) and uric acid (UA), on the electrochemical detection of dopamine were also examined. The modified electrode can successfully separate the oxidation potentials for ascorbic acid and dopamine, shifting the oxidation peak potential of ascorbic acid to a more positive potential, and significantly decreasing the peak current. The presence of ascorbic acid increased the sensitivity of dopamine determination at the modified electrode, and the detection limit was estimated to be 0.5 μM with 0.1 mM ascorbic acid to imitate physiological solutions. Additionally, studies showed that the presence of uric acid does not affect the electrochemical detection of dopamine. The modified electrode can be successfully applied for the quantitative analysis of dopamine both with and without interferents. Full article

(This article belongs to the Special Issue Mesoporous Materials: From Synthesis to Applications)

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14 pages, 3810 KiB

Open AccessArticle

Construction of a Glutathione-Responsive and Silica-Based Nanocomposite for Controlled Release of Chelator Dimercaptosuccinic Acid

by Hongqiang Zhai, Yuli Wang, Menghua Wang, Shuai Liu, Feifei Yu, Chunsheng Gao, Guiling Li and Qiang Wu

Int. J. Mol. Sci. 2018, 19(12), 3790; https://doi.org/10.3390/ijms19123790 - 28 Nov 2018

Cited by 15 | Viewed by 4453

Abstract

Dimercaptosuccinic acid (DMSA) is an oral heavy metal chelator. Although DMSA is the most acceptable chelator in the urinary excretion of toxic elements from children and adults, its defects in plasma binding and the membrane permeability limit its interaction with intracellular elements and affect its efficacy in chelation therapy. Herein, a novel nanocomposite composed of mesoporous silica nanoparticles (MSNs), disulfide bond, and DMSA was synthesized and characterized with a scanning/transmission electron microscope, IR and Raman spectra, and TGA analysis. The in vitro interactions with glutathione (GSH) and cellular uptake assays showed that it was able to be stable in extracellular environments such as in blood, be internalized by cells, and release DMSA inside via GSH-triggered disulfide cleavage reaction. The in vitro adsorption assays showed that MSNs-SH as its intracellular metabolite had strong adsorbability for models of Hg²⁺ or Pb²⁺. The hemolysis and cell viability assays showed that it was compatible with blood and cells even at a concentration of 1000 μg·mL⁻¹. All above could not only enable it to be a GSH-responsive drug delivery system (DDS) for DMSA delivery but also to be a solution for its defects and efficacy. Thus, introduction of intelligent DDS might open a new avenue for DMSA-based chelation therapy. Full article

(This article belongs to the Special Issue Mesoporous Materials: From Synthesis to Applications)

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13 pages, 2559 KiB

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Uptake and Distribution of Fenoxanil-Loaded Mesoporous Silica Nanoparticles in Rice Plants

by Feng Zhu, Xingang Liu, Lidong Cao, Chong Cao, Fengmin Li, Caijun Chen, Chunli Xu, Qiliang Huang and Fengpei Du

Int. J. Mol. Sci. 2018, 19(10), 2854; https://doi.org/10.3390/ijms19102854 - 20 Sep 2018

Cited by 38 | Viewed by 6195

Abstract

Mesoporous silica nanoparticles (MSNs) can be used as carriers to deliver pesticides into plants, which is considered to be one method of improving the efficacy of pesticide usage in agricultural production. In the present work, MSNs with an average diameter of 258.1 nm were synthesized and loaded with Fenoxanil. The structure of the nanocarriers was observed by scanning electron microscopy. The loading content of Fenoxanil-loaded MSNs was investigated. After rice plants in a hydroponic system were treated with loaded MSNs, the concentrations of Fenoxanil in different samples were determined using high-performance liquid chromatography–tandem mass spectrometry. The results suggested that rice plants can absorb MSNs from water through their roots, and the dosage has almost no effect on the distribution of Fenoxanil in rice plants. The application of pesticide-loaded nanoparticles in a hydroponic system poses a low risk of Fenoxanil accumulation in rice. Full article

(This article belongs to the Special Issue Mesoporous Materials: From Synthesis to Applications)

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