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Pharmaceutics
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Porous Inorganic Drug Delivery Systems
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Porous Inorganic Drug Delivery Systems

A special issue of Pharmaceutics (ISSN 1999-4923).

Deadline for manuscript submissions: closed (31 October 2018) | Viewed by 66957

Special Issue Editor

Prof. Dr. Nikolaos Bouropoulos

E-Mail Website
Guest Editor
1. Department of Materials Science, University of Patras, GR 26504 Patras, Greece
2. Institute of Chemical Engineering Sciences (FORTH/ICE-HT), GR 26504 Patras, Greece
Interests: biomaterials; gels; calcium phosphates; biomineralization; alginates; zinc oxide; calcium oxalate
Special Issues, Collections and Topics in MDPI journals

Special Issue Information

Dear Colleagues,

In recent years, there has been considerable interest in the development of controlled drug delivery systems that are based on inorganic porous materials. In particular, mesoporous silica nanoparticles, zeolites mesoporous bioactive glasses, etc., have been used as promising carriers for drug delivery applications. According to IUPAC nomenclature, solid materials are classified as microporous (pore diameter less than 2 nm), mesoporous (pores are between 2 and 50 nm) and macroporous (pores greater than 50 nm). The main features of porous materials are the large surface area, their pore size and pore architecture, and their floating ability in biological media. Porous matrices can increase the solubility and bioavailability of poorly soluble drugs. Factors influencing the drug release mechanism include the pore size, interactions between the drug and the host network and stabilization of the amorphous drug phase. The aim of this Special Issue is to review the current research on inorganic materials as drug delivery systems.

Prof. Bouropoulos Nikolaos
Guest Editor

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Keywords

  • zeolites
  • porous carbon materials
  • mesoporous silica nanoparticles
  • mesoporous bioactive glasses
  • porous bioceramics
  • inorganic clays
  • inorganic aerogels
  • porous Silicon
  • drug delivery systems
  • drug loading
  • pharmaceutical nanotechnology

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Published Papers (10 papers)

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Research

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14 pages, 26004 KiB  
Article
Loading of Porous Functionalized Calcium Carbonate Microparticles: Distribution Analysis with Focused Ion Beam Electron Microscopy and Mercury Porosimetry
by Maryam Farzan, Roger Roth, Gabriela Québatte, Joachim Schoelkopf, Jörg Huwyler and Maxim Puchkov
Pharmaceutics 2019, 11(1), 32; https://doi.org/10.3390/pharmaceutics11010032 - 15 Jan 2019
Cited by 15 | Viewed by 4310
Abstract
Accurate analysis of intraparticle distribution of substances within porous drug carriers is important to optimize loading and subsequent processing. Mercury intrusion porosimetry, a common technique used for characterization of porous materials, assumes cylindrical pore geometry, which may lead to misinterpretation. Therefore, imaging techniques [...] Read more.
Accurate analysis of intraparticle distribution of substances within porous drug carriers is important to optimize loading and subsequent processing. Mercury intrusion porosimetry, a common technique used for characterization of porous materials, assumes cylindrical pore geometry, which may lead to misinterpretation. Therefore, imaging techniques such as focused ion beam scanning electron microscopy (FIB-SEM) help to better interpret these results. The purpose of this study was to investigate the differences between mercury intrusion and scanning electron microscopy and to identify the limitations of each method. Porous microparticles, functionalized calcium carbonate, were loaded with bovine serum albumin and dipalmitoylphosphatidylcholine (DPPC) by solvent evaporation and results of the pore size distribution obtained by both methods were compared. The internal structure of the novel pharmaceutical excipient, functionalized calcium carbonate, was revealed for the first time. Our results demonstrated that image analysis provides a closer representation of the material distribution since it was possible to discriminate between blocked and filled pores. The physical nature of the loaded substances is critical for the deposition within the pores of functionalized calcium carbonate. We conclude, that a combination of mercury intrusion porosimetry and focused ion beam scanning electron microscopy allows for a reliable analysis of sub-micron porous structures of particulate drug carriers. Full article
(This article belongs to the Special Issue Porous Inorganic Drug Delivery Systems)
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18 pages, 2928 KiB  
Article
Preparation and Study of the Antibacterial Applications and Oxidative Stress Induction of Copper Maleamate-Functionalized Mesoporous Silica Nanoparticles
by Diana Díaz-García, Perla R. Ardiles, Sanjiv Prashar, Antonio Rodríguez-Diéguez, Paulina L. Páez and Santiago Gómez-Ruiz
Pharmaceutics 2019, 11(1), 30; https://doi.org/10.3390/pharmaceutics11010030 - 14 Jan 2019
Cited by 45 | Viewed by 4597
Abstract
Mesoporous silica nanoparticles (MSNs) are an interesting class of nanomaterials with potential applications in different therapeutic areas and that have been extensively used as drug carriers in different fields of medicine. The present work is focused on the synthesis of MSNs containing a [...] Read more.
Mesoporous silica nanoparticles (MSNs) are an interesting class of nanomaterials with potential applications in different therapeutic areas and that have been extensively used as drug carriers in different fields of medicine. The present work is focused on the synthesis of MSNs containing a maleamato ligand (MSN-maleamic) and the subsequent coordination of copper(II) ions (MSN-maleamic-Cu) for the exploration of their potential application as antibacterial agents. The Cu-containing nanomaterials have been characterized by different techniques and the preliminary antibacterial effect of the supported maleamato-copper(II) complexes has been tested against two types of bacteria (Gram positive and Gram negative) in different assays to determine the minimum inhibitory concentration (MIC) and minimum bactericidal concentration (MBC). The biological results showed a moderate antibacterial activity against Escherichia coli which motivated a more detailed study of the antibacterial mechanism of action of the synthesized maleamate-containing nanosystems and whose findings showed oxidative stress generation in bacterial cells. All the prepared nanomaterials were also tested as catalysts in the “solvent free” selective oxidation of benzyl alcohol, to observe if there is a potential correlation between the catalytic oxidation capacity of the materials and the observed oxidative stress in bacteria. This may help in the future, for a more accurate rational design of antibacterial nanosystems, based on their observed catalytic oxidation activity. Full article
(This article belongs to the Special Issue Porous Inorganic Drug Delivery Systems)
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16 pages, 3586 KiB  
Article
Enhanced Solubility, Permeability and Anticancer Activity of Vorinostat Using Tailored Mesoporous Silica Nanoparticles
by Anand Kumar Meka, Laura J. Jenkins, Mercedes Dàvalos-Salas, Naisarg Pujara, Kuan Yau Wong, Tushar Kumeria, John M. Mariadason and Amirali Popat
Pharmaceutics 2018, 10(4), 283; https://doi.org/10.3390/pharmaceutics10040283 - 17 Dec 2018
Cited by 51 | Viewed by 6684
Abstract
Suberoylanilide hydroxamic acid (SAHA) or vorinostat (VOR) is a potent inhibitor of class I histone deacetylases (HDACs) that is approved for the treatment of cutaneous T-cell lymphoma. However, it has the intrinsic limitations of low water solubility and low permeability which reduces its [...] Read more.
Suberoylanilide hydroxamic acid (SAHA) or vorinostat (VOR) is a potent inhibitor of class I histone deacetylases (HDACs) that is approved for the treatment of cutaneous T-cell lymphoma. However, it has the intrinsic limitations of low water solubility and low permeability which reduces its clinical potential especially when given orally. Packaging of drugs within ordered mesoporous silica nanoparticles (MSNs) is an emerging strategy for increasing drug solubility and permeability of BCS (Biopharmaceutical Classification System) class II and IV drugs. In this study, we encapsulated vorinostat within MSNs modified with different functional groups, and assessed its solubility, permeability and anti-cancer efficacy in vitro. Compared to free drug, the solubility of vorinostat was enhanced 2.6-fold upon encapsulation in pristine MSNs (MCM-41-VOR). Solubility was further enhanced when MSNs were modified with silanes having amino (3.9 fold) or phosphonate (4.3 fold) terminal functional groups. Moreover, permeability of vorinostat into Caco-2 human colon cancer cells was significantly enhanced for MSN-based formulations, particularly MSNs modified with amino functional group (MCM-41-NH2-VOR) where it was enhanced ~4 fold. Compared to free drug, vorinostat encapsulated within amino-modified MSNs robustly induced histone hyperacetylation and expression of established histone deacetylase inhibitor (HDACi)-target genes, and induced extensive apoptosis in HCT116 colon cancer cells. Similar effects were observed on apoptosis induction in HH cutaneous T-cell lymphoma cells. Thus, encapsulation of the BCS class IV molecule vorinostat within MSNs represents an effective strategy for improving its solubility, permeability and anti-tumour activity. Full article
(This article belongs to the Special Issue Porous Inorganic Drug Delivery Systems)
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18 pages, 4461 KiB  
Article
Factors Affecting Intracellular Delivery and Release of Hydrophilic Versus Hydrophobic Cargo from Mesoporous Silica Nanoparticles on 2D and 3D Cell Cultures
by Diti Desai, Malin Åkerfelt, Neeraj Prabhakar, Mervi Toriseva, Tuomas Näreoja, Jixi Zhang, Matthias Nees and Jessica M. Rosenholm
Pharmaceutics 2018, 10(4), 237; https://doi.org/10.3390/pharmaceutics10040237 - 17 Nov 2018
Cited by 10 | Viewed by 5339
Abstract
Intracellular drug delivery by mesoporous silica nanoparticles (MSNs) carrying hydrophilic and hydrophobic fluorophores as model drug cargo is demonstrated on 2D cellular and 3D tumor organoid level. Two different MSN designs, chosen on the basis of the characteristics of the loaded cargo, were [...] Read more.
Intracellular drug delivery by mesoporous silica nanoparticles (MSNs) carrying hydrophilic and hydrophobic fluorophores as model drug cargo is demonstrated on 2D cellular and 3D tumor organoid level. Two different MSN designs, chosen on the basis of the characteristics of the loaded cargo, were used: MSNs with a surface-grown poly(ethylene imine), PEI, coating only for hydrophobic cargo and MSNs with lipid bilayers covalently coupled to the PEI layer as a diffusion barrier for hydrophilic cargo. First, the effect of hydrophobicity corresponding to loading degree (hydrophobic cargo) as well as surface charge (hydrophilic cargo) on intracellular drug release was studied on the cellular level. All incorporated agents were able to release to varying degrees from the endosomes into the cytoplasm in a loading degree (hydrophobic) or surface charge (hydrophilic) dependent manner as detected by live cell imaging. When administered to organotypic 3D tumor models, the hydrophilic versus hydrophobic cargo-carrying MSNs showed remarkable differences in labeling efficiency, which in this case also corresponds to drug delivery efficacy in 3D. The obtained results could thus indicate design aspects to be taken into account for the development of efficacious intracellular drug delivery systems, especially in the translation from standard 2D culture to more biologically relevant organotypic 3D cultures. Full article
(This article belongs to the Special Issue Porous Inorganic Drug Delivery Systems)
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14 pages, 5008 KiB  
Article
Fabrication and Characterization of Strontium-Substituted Hydroxyapatite-CaO-CaCO3 Nanofibers with a Mesoporous Structure as Drug Delivery Carriers
by Shiao-Wen Tsai, Wen-Xin Yu, Pai-An Hwang, Sheng-Siang Huang, Hsiu-Mei Lin, Yu-Wei Hsu and Fu-Yin Hsu
Pharmaceutics 2018, 10(4), 179; https://doi.org/10.3390/pharmaceutics10040179 - 8 Oct 2018
Cited by 40 | Viewed by 5315
Abstract
Hydroxyapatite (HAp) is the main inorganic component and an essential part of hard bone and teeth. Due to its excellent biocompatibility, bioactivity, and osteoconductivity, synthetic HAp has been widely used as a bone substitute, cell carrier, and therapeutic gene or drug carrier. Recently, [...] Read more.
Hydroxyapatite (HAp) is the main inorganic component and an essential part of hard bone and teeth. Due to its excellent biocompatibility, bioactivity, and osteoconductivity, synthetic HAp has been widely used as a bone substitute, cell carrier, and therapeutic gene or drug carrier. Recently, numerous studies have demonstrated that strontium-substituted hydroxyapatite (SrHAp) not only enhances osteogenesis but also inhibits adipogenesis in mesenchymal stem cells. Mesoporous SrHAp has been successfully synthesized via a traditional template-based process and has been found to possess better drug loading and release efficiencies than SrHAp. In this study, strontium-substituted hydroxyapatite-CaO-CaCO3 nanofibers with a mesoporous structure (mSrHANFs) were fabricated using a sol–gel method followed by electrospinning. X-ray diffraction analysis revealed that the contents of CaO and CaCO3 in the mSrHANFs decreased as the doping amount of Sr increased. Scanning electron microscopy (SEM) images showed that the average diameter of the mSrHANFs was approximately 200~300 nm. The N2 adsorption–desorption isotherms demonstrated that the mSrHANFs possessed a mesoporous structure and that the average pore size was approximately 20~25 nm. Moreover, the mSrHANFs had excellent drug- loading efficiency and could retard the burst release of tetracycline (TC) to maintain antibacterial activity for over 3 weeks. Hence, mSrHANFs have the potential to be used as drug carriers in bone tissue engineering. Full article
(This article belongs to the Special Issue Porous Inorganic Drug Delivery Systems)
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Review

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29 pages, 6394 KiB  
Review
Mesoporous Silica Materials as Drug Delivery: “The Nightmare” of Bacterial Infection
by Marina Martínez-Carmona, Yurii K. Gun’ko and María Vallet-Regí
Pharmaceutics 2018, 10(4), 279; https://doi.org/10.3390/pharmaceutics10040279 - 15 Dec 2018
Cited by 79 | Viewed by 8976
Abstract
Mesoporous silica materials (MSM) have a great surface area and a high pore volume, meaning that they consequently have a large loading capacity, and have been demonstrated to be unique candidates for the treatment of different pathologies, including bacterial infection. In this text, [...] Read more.
Mesoporous silica materials (MSM) have a great surface area and a high pore volume, meaning that they consequently have a large loading capacity, and have been demonstrated to be unique candidates for the treatment of different pathologies, including bacterial infection. In this text, we review the multiple ways of action in which MSM can be used to fight bacterial infection, including early detection, drug release, targeting bacteria or biofilm, antifouling surfaces, and adjuvant capacity. This review focus mainly on those that act as a drug delivery system, and therefore that have an essential characteristic, which is their great loading capacity. Since MSM have advantages in all stages of combatting bacterial infection; its prevention, detection and finally in its treatment, we can venture to talk about them as the “nightmare of bacteria”. Full article
(This article belongs to the Special Issue Porous Inorganic Drug Delivery Systems)
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20 pages, 1822 KiB  
Review
Drug-Loaded Biomimetic Ceramics for Tissue Engineering
by Patricia Diaz-Rodriguez, Mirian Sánchez and Mariana Landin
Pharmaceutics 2018, 10(4), 272; https://doi.org/10.3390/pharmaceutics10040272 - 13 Dec 2018
Cited by 49 | Viewed by 4908
Abstract
The mimesis of biological systems has been demonstrated to be an adequate approach to obtain tissue engineering scaffolds able to promote cell attachment, proliferation, and differentiation abilities similar to those of autologous tissues. Bioceramics are commonly used for this purpose due to their [...] Read more.
The mimesis of biological systems has been demonstrated to be an adequate approach to obtain tissue engineering scaffolds able to promote cell attachment, proliferation, and differentiation abilities similar to those of autologous tissues. Bioceramics are commonly used for this purpose due to their similarities to the mineral component of hard tissues as bone. Furthermore, biomimetic scaffolds are frequently loaded with diverse therapeutic molecules to enhance their biological performance, leading to final products with advanced functionalities. In this review, we aim to describe the already developed bioceramic-based biomimetic systems for drug loading and local controlled release. We will discuss the mechanisms used for the inclusion of therapeutic molecules on the designed systems, paying special attention to the identification of critical parameters that modulate drug loading and release kinetics on these scaffolds. Full article
(This article belongs to the Special Issue Porous Inorganic Drug Delivery Systems)
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18 pages, 1128 KiB  
Review
Dealing with Skin and Blood-Brain Barriers: The Unconventional Challenges of Mesoporous Silica Nanoparticles
by Alessandra Nigro, Michele Pellegrino, Marianna Greco, Alessandra Comandè, Diego Sisci, Luigi Pasqua, Antonella Leggio and Catia Morelli
Pharmaceutics 2018, 10(4), 250; https://doi.org/10.3390/pharmaceutics10040250 - 1 Dec 2018
Cited by 42 | Viewed by 5543
Abstract
Advances in nanotechnology for drug delivery are fostering significant progress in medicine and diagnostics. The multidisciplinary nature of the nanotechnology field encouraged the development of innovative strategies and materials to treat a wide range of diseases in a highly specific way, which allows [...] Read more.
Advances in nanotechnology for drug delivery are fostering significant progress in medicine and diagnostics. The multidisciplinary nature of the nanotechnology field encouraged the development of innovative strategies and materials to treat a wide range of diseases in a highly specific way, which allows reducing the drug dosage and, consequently, improving the patient’s compliance. Due to their good biocompatibility, easy synthesis, and high versatility, inorganic frameworks represent a valid tool to achieve this aim. In this context, Mesoporous Silica Nanoparticles (MSNs) are emerging in the biomedical field. For their ordered porosity and high functionalizable surface, achievable with an inexpensive synthesis process and being non-hazardous to biological tissues, MSNs offer ideal solutions to host, protect, and transport drugs to specific target sites. Extensive literature exists on the use of MSNs as targeted vehicles for systemic (chemo) therapy and for imaging/diagnostic purposes. However, the aim of this review is to give an overview of the last updates on the potential applications of the MSNs for Topical Drug Delivery (TDD) and as drug delivery systems into the brain, discussing their performances and advantages in dealing with these intriguing biological barriers. Full article
(This article belongs to the Special Issue Porous Inorganic Drug Delivery Systems)
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15 pages, 2975 KiB  
Review
Diatoms Green Nanotechnology for Biosilica-Based Drug Delivery Systems
by Monica Terracciano, Luca De Stefano and Ilaria Rea
Pharmaceutics 2018, 10(4), 242; https://doi.org/10.3390/pharmaceutics10040242 - 20 Nov 2018
Cited by 83 | Viewed by 9835
Abstract
Diatom microalgae are the most outstanding natural source of porous silica. The diatom cell is enclosed in a three-dimensional (3-D) ordered nanopatterned silica cell wall, called frustule. The unique properties of the diatom frustule, including high specific surface area, thermal stability, biocompatibility, and [...] Read more.
Diatom microalgae are the most outstanding natural source of porous silica. The diatom cell is enclosed in a three-dimensional (3-D) ordered nanopatterned silica cell wall, called frustule. The unique properties of the diatom frustule, including high specific surface area, thermal stability, biocompatibility, and tailorable surface chemistry, make diatoms really promising for biomedical applications. Moreover, they are easy to cultivate in an artificial environment and there is a large availability of diatom frustules as fossil material (diatomite) in several areas of the world. For all these reasons, diatoms are an intriguing alternative to synthetic materials for the development of low-cost drug delivery systems. This review article focuses on the possible use of diatom-derived silica as drug carrier systems. The functionalization strategies of diatom micro/nanoparticles for improving their biophysical properties, such as cellular internalization and drug loading/release kinetics, are described. In addition, the realization of hybrid diatom-based devices with advanced properties for theranostics and targeted or augmented drug delivery applications is also discussed. Full article
(This article belongs to the Special Issue Porous Inorganic Drug Delivery Systems)
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35 pages, 4340 KiB  
Review
Porous Inorganic Carriers Based on Silica, Calcium Carbonate and Calcium Phosphate for Controlled/Modulated Drug Delivery: Fresh Outlook and Future Perspectives
by Alexey D. Trofimov, Anna A. Ivanova, Mikhail V. Zyuzin and Alexander S. Timin
Pharmaceutics 2018, 10(4), 167; https://doi.org/10.3390/pharmaceutics10040167 - 25 Sep 2018
Cited by 112 | Viewed by 10223
Abstract
Porous inorganic nanostructured materials are widely used nowadays as drug delivery carriers due to their adventurous features: suitable architecture, large surface area and stability in the biological fluids. Among the different types of inorganic porous materials, silica, calcium carbonate, and calcium phosphate have [...] Read more.
Porous inorganic nanostructured materials are widely used nowadays as drug delivery carriers due to their adventurous features: suitable architecture, large surface area and stability in the biological fluids. Among the different types of inorganic porous materials, silica, calcium carbonate, and calcium phosphate have received significant attention in the last decade. The use of porous inorganic materials as drug carriers for cancer therapy, gene delivery etc. has the potential to improve the life expectancy of the patients affected by the disease. The main goal of this review is to provide general information on the current state of the art of synthesis of the inorganic porous particles based on silica, calcium carbonate and calcium phosphate. Special focus is dedicated to the loading capacity, controllable release of drugs under internal biological stimuli (e.g., pH, redox, enzymes) and external noninvasive stimuli (e.g., light, magnetic field, and ultrasound). Moreover, the diverse compounds to deliver with silica, calcium carbonate and calcium phosphate particles, ranging from the commercial drugs to genetic materials are also discussed. Full article
(This article belongs to the Special Issue Porous Inorganic Drug Delivery Systems)
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