Functionalized Porous Silica-Based Nanoparticles: From Synthesis to Applications

A special issue of Nanomaterials (ISSN 2079-4991). This special issue belongs to the section "Synthesis, Interfaces and Nanostructures".

Deadline for manuscript submissions: closed (31 August 2020) | Viewed by 44930

Special Issue Editor

CIBER de Bioingeniería, Biomateriales y Nanomedicina (CIBER-BBN) and Instituto Interuniversitario de Investigación de Reconocimiento Molecular y Desarrollo Tecnológico (IDM), Universitat Politècnica de València-Universitat de València, Camino de Vera s/n, 46022 Valencia, Spain
Interests: functional mesoporous materials; controlled release applications; nanotherapies; nanodiagnostics; smart nanomaterials

Special Issue Information

Dear Colleagues,

Porous silica-based nanoparticles are one of the most commonly-used supports to prepare functional nanomaterials. In general, these materials are synthesized using a self-assembly strategy based on the hydrolysis of an inorganic precursor around a pre-organized organic template such as surfactant micelles or block copolymers. The obtained supports can be easily chemically-modified as silicon oxide functionalization chemistry has been widely studied. At present, it is possible to modulate density, distribution, or even the location of the incorporated functional groups. Decoration of these materials with molecules, super-molecules or even with other inorganic materials confers new advantageous features to the final material, which find application in many fields, such as controlled release, molecular and biomolecular recognition, imaging, self-healing, remediation, catalysis or biomaterials among others. The present Special Issue is focused on the preparation and applications of new functional hybrid silica-based nanomaterials. This is a timely topic of research and an increasing interest in this kind of nanomaterials is envisioned due to their potential broad application in many fields.

Dr. Elena Aznar
Guest Editor

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Keywords

  • Functional porous materials
  • Silica
  • Nanoparticles
  • Porous silica-based nanoparticles and controlled release
  • Porous silica-based nanoparticles and biomedical applications
  • Porous silica-based nanoparticles and self-healing
  • Porous silica-based nanoparticles and remediation
  • Porous silica-based nanoparticles and catalysis

Published Papers (11 papers)

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Research

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24 pages, 5351 KiB  
Article
Incorporation of Manganese Complexes within Hybrid Resol-Silica and Carbon-Silica Nanoparticles
by François-Xavier Turquet, Montserrat Corbella, Clémentine Fellah, Gilles Montagnac, Bruno Reynard, Laurent Bonneviot, Kun Zhang and Belén Albela
Nanomaterials 2021, 11(3), 774; https://doi.org/10.3390/nano11030774 - 18 Mar 2021
Viewed by 1754
Abstract
The incorporation of a luminescent probe into a nano-vector is one of the approaches used to design chemosensors and nanocargos for drug delivery and theranostics. The location of the nano-vector can be followed using fluorescence spectroscopy together with the change of environment that [...] Read more.
The incorporation of a luminescent probe into a nano-vector is one of the approaches used to design chemosensors and nanocargos for drug delivery and theranostics. The location of the nano-vector can be followed using fluorescence spectroscopy together with the change of environment that affects the fluorescence properties. The ligand 9-anthracene carboxylate is proposed in this study as a luminescent probe to locate two types of manganese complexes inside three series of porous nanoparticles of different composition: resol-silica, carbon-silica and pure silica. The manganese complexes are a tetranuclear MnIII cluster [MnIII4(μ-O)2(μ-AntCO2)6(bpy)2(ClO4)2] with a butterfly core, and a MnII dinuclear complex [{MnII(bpy)(AntCO2)}2(μ-AntCO2)2(μ-OH2)]. The magnetic measurements indicate that both complexes are present as dinuclear entities when incorporated inside the particles. Both the Mn complexes and the nanoparticles are luminescent. However, when the metal complexes are introduced into the nanoparticles, the luminescent properties of both are altered. The study of the fluorescence of the nanoparticles’ suspensions and of the supernatants shows that MnII compounds seem to be more retained inside the particles than MnIII compounds. The resol-silica nanoparticles with MnII complexes inside is the material that presents the lowest complex leaching in ethanol. Full article
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11 pages, 2120 KiB  
Article
Use of Silica Based Materials as Modulators of the Lipase Catalyzed Hydrolysis of Fats under Simulated Duodenal Conditions
by Sara Muñoz-Pina, Pedro Amorós, Jamal El Haskouri, Ana Andrés and José V. Ros-Lis
Nanomaterials 2020, 10(10), 1927; https://doi.org/10.3390/nano10101927 - 27 Sep 2020
Cited by 3 | Viewed by 1989
Abstract
The effect of silica materials and their functionalization in the lipase catalyzed fat hydrolysis has been scarcely studied. Fifteen silica materials were prepared and their effect on the fat hydrolysis was measured, under simulated duodenal conditions, using the pH-stat method. The materials are [...] Read more.
The effect of silica materials and their functionalization in the lipase catalyzed fat hydrolysis has been scarcely studied. Fifteen silica materials were prepared and their effect on the fat hydrolysis was measured, under simulated duodenal conditions, using the pH-stat method. The materials are composed of the combination of three supports (Stöber massive silica nanoparticles, Stöber mesoporous nanoparticles and UVM-7) and four surface functionalizations (methyl, trimethyl, propyl and octyl). In addition, the non-functionalized materials were tested. The functional groups were selected to offer a hydrophobic character to the material improving the interaction with the fat globules and the lipase. The materials are able to modulate the lipase activity and their effect depending on the support topology and the organic covering, being able to increase or reduce the fat hydrolysis. Depending of the material, relative fat hydrolysis rates of 75 to 140% in comparison with absence of the material were obtained. The results were analyzed by Partial Least Square Regression and suggest that the alkyl modified mesopores are able to improve the fat hydrolysis, by contrast the non-porous nanoparticles and the textural pores tend to induce inhibition. The effects are more pronounced for materials containing long alkyl chains and/or in absence of taurodeoxycholate. Full article
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18 pages, 3629 KiB  
Article
Surfactant-Triggered Molecular Gate Tested on Different Mesoporous Silica Supports for Gastrointestinal Controlled Delivery
by Elisa Poyatos-Racionero, Isabel González-Álvarez, Marta González-Álvarez, Ramón Martínez-Máñez, M. Dolores Marcos, Andrea Bernardos and Elena Aznar
Nanomaterials 2020, 10(7), 1290; https://doi.org/10.3390/nano10071290 - 30 Jun 2020
Cited by 9 | Viewed by 2238
Abstract
In recent decades, the versatility of mesoporous silica particles and their relevance to develop controlled release systems have been demonstrated. Within them, gated materials able to modulate payload delivery represent great advantages. However, the role played by the porous matrix in this kind [...] Read more.
In recent decades, the versatility of mesoporous silica particles and their relevance to develop controlled release systems have been demonstrated. Within them, gated materials able to modulate payload delivery represent great advantages. However, the role played by the porous matrix in this kind of systems is scarce. In this work, different mesoporous silica materials (MCM-41, MCM-48, SBA-15 and UVM-7) are functionalized with oleic acid as a molecular gate. All systems are fully characterized and their ability to confine the entrapped cargo and release it in the presence of bile salts is validated with release assays and in vitro digestion experiments. The cargo release profile of each synthesized support is studied, paying attention to the inorganic scaffold. Obtained release profiles fit to Korsmeyer–Peppas model, which explains the differences among the studied supports. Based on the results, UVM-7 material was the most appropriate system for duodenal delivery and was tested in an in vivo model of the Wistar rat. Payload confinement and its complete release after gastric emptying is achieved, establishing the possible use of mesoporous silica particles as protection and direct release agents into the duodenum and, hence, demonstrating that these systems could serve as an alternative to the administration methods employed until now. Full article
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14 pages, 3470 KiB  
Article
Hafnium-Doped Mesoporous Silica as Efficient Lewis Acidic Catalyst for Friedel–Crafts Alkylation Reactions
by Yao-Bing Huang, Yu-Jia Luo and Fei Wang
Nanomaterials 2019, 9(8), 1128; https://doi.org/10.3390/nano9081128 - 05 Aug 2019
Cited by 13 | Viewed by 3276
Abstract
The development of an efficient solid catalyst for Friedel–Crafts (FC) reactions is of great importance to organic synthetic chemistry. Herein, we reported the hafnium-doped mesoporous silica catalyst Hf/SBA-15 and its first use for Friedel–Crafts alkylation reactions. Catalysts with different Si/Hf ratios were prepared [...] Read more.
The development of an efficient solid catalyst for Friedel–Crafts (FC) reactions is of great importance to organic synthetic chemistry. Herein, we reported the hafnium-doped mesoporous silica catalyst Hf/SBA-15 and its first use for Friedel–Crafts alkylation reactions. Catalysts with different Si/Hf ratios were prepared and characterized, among which Hf/SBA-15(20) (Si/Hf = 20:1) was the most active catalyst, offering up to 99.1% benzylated product under mild reaction conditions. The influences of reaction conditions on the product were systematically investigated and compared. Pyridine-IR characterization of the catalyst showed that Lewis acid formed the primary active sites for the Friedel–Crafts alkylation reaction. X-ray photoelectron spectroscopy (XPS) characterization revealed that the electron shift from the Hf center to the silica framework resulted in a more active Lewis metal center for FC reactions. Moreover, the catalyst was successfully applied to the alkylation reaction with different alcohols and aromatic compounds. Finally, the Hf/SBA-15(20) catalyst also showed good recyclability in the recycling runs, demonstrating its high potential of being used for large scale FC reactions in the industry. Full article
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13 pages, 2058 KiB  
Article
Hybrid Mesoporous Nanoparticles for pH-Actuated Controlled Release
by José L. M. Gonçalves, Carina I. C. Crucho, Sérgio P. C. Alves, Carlos Baleizão and José Paulo S. Farinha
Nanomaterials 2019, 9(3), 483; https://doi.org/10.3390/nano9030483 - 26 Mar 2019
Cited by 14 | Viewed by 4125
Abstract
Among a variety of inorganic-based nanomaterials, mesoporous silica nanoparticles (MSNs) have several attractive features for application as a delivery system, due to their high surface areas, large pore volumes, uniform and tunable pore sizes, high mechanical stability, and a great diversity of surface [...] Read more.
Among a variety of inorganic-based nanomaterials, mesoporous silica nanoparticles (MSNs) have several attractive features for application as a delivery system, due to their high surface areas, large pore volumes, uniform and tunable pore sizes, high mechanical stability, and a great diversity of surface functionalization options. We developed novel hybrid MSNs composed of a mesoporous silica nanostructure core and a pH-responsive polymer shell. The polymer shell was prepared by RAFT polymerization of 2-(diisopropylamino)ethyl methacrylate (pKa ~6.5), using a hybrid grafting approach. The hybrid nanoparticles have diameters of ca. 100 nm at pH < 6.5 and ca. 60 nm at pH > 6.5. An excellent control of cargo release is achieved by the combined effect of electrostatic interaction of the cargo with the charged silica and the extended cationic polymer chains at low pH, and the reduction of electrostatic attraction with a simultaneous collapse of the polymer chains to a globular conformation at higher pH. The system presents a very low (almost null) release rate at acidic pH values and a large release rate at basic pH, resulting from the squeezing-out effect of the coil-to-globule transition in the polymer shell. Full article
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17 pages, 3038 KiB  
Article
A Study of Catalytic Oxidation of a Library of C2 to C4 Alcohols in the Presence of Nanogold
by Maciej Kapkowski, Anna Niemczyk-Wojdyla, Piotr Bartczak, Monika Pyrkosz Bulska, Kamila Gajcy, Rafal Sitko, Maciej Zubko, Jacek Szade, Joanna Klimontko, Katarzyna Balin and Jaroslaw Polanski
Nanomaterials 2019, 9(3), 442; https://doi.org/10.3390/nano9030442 - 15 Mar 2019
Cited by 1 | Viewed by 2893
Abstract
The classical stoichiometric oxidation of alcohols is an important tool in contemporary organic chemistry. However, it still requires huge modifications in order to comply with the principles of green chemistry. The use of toxic chemicals, hazardous organic solvents, and the large amounts of [...] Read more.
The classical stoichiometric oxidation of alcohols is an important tool in contemporary organic chemistry. However, it still requires huge modifications in order to comply with the principles of green chemistry. The use of toxic chemicals, hazardous organic solvents, and the large amounts of toxic wastes that result from the reactions are a few examples of the problems that must be solved. Nanogold alone or conjugated with palladium were supported on different carriers (SiO2, C) and investigated in order to evaluate their catalytic potential for environmentally friendly alcohol oxidation under solvent-free and base-free conditions in the presence H2O2 as a clean oxidant. We tested different levels of Au loading (0.1–1.2% wt.) and different active catalytic site forms (monometallic Au or bimetallic Au–Pd sites). This provided new insights on how the structure of the Au-dispersions affected their catalytic performance. Importantly, the examination of the catalytic performance of the resulting catalysts was oriented toward a broad scope of alcohols, including those that are the most resistant to oxidation—the primary aliphatic alcohols. Surprisingly, the studies proved that Au/SiO2 at a level of Au loading as low as 0.1% wt. appeared to be efficient and prospective catalytic system for the green oxidation of alcohol. Most importantly, the results revealed that 0.1% Au/SiO2 might be the catalyst of choice with a wide scope of utility in the green oxidation of various structurally different alcohols as well as the non-activated aliphatic ones. Full article
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13 pages, 7107 KiB  
Article
Tailored Synthesis of Core-Shell Mesoporous Silica Particles—Optimization of Dye Sorption Properties
by Andrzej Baliś and Szczepan Zapotoczny
Nanomaterials 2018, 8(4), 230; https://doi.org/10.3390/nano8040230 - 10 Apr 2018
Cited by 13 | Viewed by 4454
Abstract
Monodisperse spherical silica particles, with solid cores and mesoporous shells (SCMS), were synthesized at various temperatures using a one-pot method utilizing a cationic surfactant template. The temperature of the synthesis was found to significantly affect the diameters of both the cores (ca. 170–800 [...] Read more.
Monodisperse spherical silica particles, with solid cores and mesoporous shells (SCMS), were synthesized at various temperatures using a one-pot method utilizing a cationic surfactant template. The temperature of the synthesis was found to significantly affect the diameters of both the cores (ca. 170–800 nm) and shells (ca. 11–80 nm) of the particles, which can be tailored for specific applications that require a high specific surface area of the nanocarriers (mesoporous shells) and simultaneously their mechanical robustness for, e.g., facile isolation from suspensions (dense cores). The applied method enabled the formation of the relatively thick mesoporous shells at conditions below room temperature. Radially ordered pores with narrow distributions of their sizes in 3–4 nm range were found in the shells. The adsorption ability of the SCMS particles was studied using rhodamine 6G as a model dye. Decolorization of the dye solution in the presence of the SCMS particles was correlated with their structure and specific surface area and reached its maximum for the particles synthesized at 15 °C. The presented strategy may be applied for the fine-tuning of the structure of SCMS particles and the enhancement of their adsorption capabilities. Full article
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Review

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49 pages, 4114 KiB  
Review
Influence of the Surface Functionalization on the Fate and Performance of Mesoporous Silica Nanoparticles
by Miguel Gisbert-Garzarán and María Vallet-Regí
Nanomaterials 2020, 10(5), 916; https://doi.org/10.3390/nano10050916 - 09 May 2020
Cited by 45 | Viewed by 6126
Abstract
Mesoporous silica nanoparticles have been broadly applied as drug delivery systems owing to their exquisite features, such as excellent textural properties or biocompatibility. However, there are various biological barriers that prevent their proper translation into the clinic, including: (1) lack of selectivity toward [...] Read more.
Mesoporous silica nanoparticles have been broadly applied as drug delivery systems owing to their exquisite features, such as excellent textural properties or biocompatibility. However, there are various biological barriers that prevent their proper translation into the clinic, including: (1) lack of selectivity toward tumor tissues, (2) lack of selectivity for tumoral cells and (3) endosomal sequestration of the particles upon internalization. In addition, their open porous structure may lead to premature drug release, consequently affecting healthy tissues and decreasing the efficacy of the treatment. First, this review will provide a comprehensive and systematic overview of the different approximations that have been implemented into mesoporous silica nanoparticles to overcome each of such biological barriers. Afterward, the potential premature and non-specific drug release from these mesoporous nanocarriers will be addressed by introducing the concept of stimuli-responsive gatekeepers, which endow the particles with on-demand and localized drug delivery. Full article
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18 pages, 6421 KiB  
Review
Recent Studies on Fluorinated Silica Nanometer-Sized Particles
by Scott T. Iacono and Abby R. Jennings
Nanomaterials 2019, 9(5), 684; https://doi.org/10.3390/nano9050684 - 02 May 2019
Cited by 13 | Viewed by 4655
Abstract
Since initially being reported, fluorinated silica nanometer-sized particles (F-SiNPs) have gained much interest in the scientific community, due to their unique properties. These properties, include, low surface energies, increased mechanical strength, thermal robustness, and chemical resistance, and are a direct result of the [...] Read more.
Since initially being reported, fluorinated silica nanometer-sized particles (F-SiNPs) have gained much interest in the scientific community, due to their unique properties. These properties, include, low surface energies, increased mechanical strength, thermal robustness, and chemical resistance, and are a direct result of the incorporation of fluorine with a nanometer-sized silica network. This review aims to summarize the synthetic methods that have, and are still, being utilized to prepare these specialized materials. Following this, applications for F-SiNPs, with an emphasis on recent examples, will be presented in further detail. Full article
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23 pages, 5387 KiB  
Review
Smart Mesoporous Silica Nanoparticles for Protein Delivery
by Hai-Jun Liu and Peisheng Xu
Nanomaterials 2019, 9(4), 511; https://doi.org/10.3390/nano9040511 - 02 Apr 2019
Cited by 54 | Viewed by 7460
Abstract
Mesoporous silica nanoparticles (MSN) have attracted a lot of attention during the past decade which is attributable to their versatile and high loading capacity, easy surface functionalization, excellent biocompatibility, and great physicochemical and thermal stability. In this review, we discuss the factors affecting [...] Read more.
Mesoporous silica nanoparticles (MSN) have attracted a lot of attention during the past decade which is attributable to their versatile and high loading capacity, easy surface functionalization, excellent biocompatibility, and great physicochemical and thermal stability. In this review, we discuss the factors affecting the loading of protein into MSN and general strategies for targeted delivery and controlled release of proteins with MSN. Additionally, we also give an outlook for the remaining challenges in the clinical translation of protein-loaded MSNs. Full article
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26 pages, 5399 KiB  
Review
Functionalized Porous Silica-Based Nano/Micro Particles for Environmental Remediation of Hazard Ions
by Chun Min Li, Xin Peng Wang, Zi Hao Jiao, Yu Sheng Zhang, Xiang Biao Yin, Xue Min Cui and Yue Zhou Wei
Nanomaterials 2019, 9(2), 247; https://doi.org/10.3390/nano9020247 - 12 Feb 2019
Cited by 32 | Viewed by 5009
Abstract
The adsorption and separation of hazard metal ions, radioactive nuclides, or minor actinides from wastewater and high-level radioactive waste liquids using functional silica-based nano/micro-particles modified with various inorganic materials or organic groups, has attracted significant attention since the discovery of ordered mesoporous silica-based [...] Read more.
The adsorption and separation of hazard metal ions, radioactive nuclides, or minor actinides from wastewater and high-level radioactive waste liquids using functional silica-based nano/micro-particles modified with various inorganic materials or organic groups, has attracted significant attention since the discovery of ordered mesoporous silica-based substrates. Focusing on inorganic and organic modified materials, the synthesis methods and sorption performances for specific ions in aqueous solutions are summarized in this review. Three modification methods for silica-based particles, the direct synthesis method, wetness impregnation method, and layer-by-layer (LBL) deposition, are usually adopted to load inorganic material onto silica-based particles, while the wetness impregnation method is currently used for the preparation of functional silica-based particles modified with organic groups. Generally, the specific synthesis method is employed based on the properties of the loading materials and the silicon-based substrate. Adsorption of specific toxic ions onto modified silica-based particles depends on the properties of the loaded material. The silicon matrix only changes the thermodynamic and mechanical properties of the material, such as the abrasive resistance, dispersibility, and radiation resistance. In this paper, inorganic loads, such as metal phosphates, molybdophosphate, titanate-based materials, and hydrotalcite, in addition to organic loads, such as 1,3-[(2,4-diethylheptylethoxy)oxy]-2,4-crown-6-Calix{4}arene (Calix {4}) arene-R14 and functional 2,6-bis-(5,6-dialkyl-1,2,4-triazin-3-yl)-pyridines(BTP) are reviewed. More specifically, we emphasize on the synthesis methods of such materials, their structures in relation to their capacities, their selectivities for trapping specific ions from either single or multi-component aqueous solutions, and the possible retention mechanisms. Potential candidates for remediation uses are selected based on their sorption capacities and distribution coefficients for target cations and the pH window for an optimum cation capture. Full article
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