Materials

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10 pages, 1819 KiB

Open AccessArticle

Extended Polysaccharide Analysis within the Liposomal Encapsulation of Polysaccharides System

by Roozbeh Nayerhoda, Dongwon Park, Charles Jones, Elsa N. Bou Ghanem and Blaine A. Pfeifer

Materials 2020, 13(15), 3320; https://doi.org/10.3390/ma13153320 - 26 Jul 2020

Cited by 2 | Viewed by 4099

The Liposomal Encapsulation of Polysaccharides (LEPS) dual antigen vaccine carrier system was assessed across two distinct polysaccharides for encapsulation efficiency, subsequent liposomal surface adornment with protein, adjuvant addition, and size and charge metrics. The polysaccharides derive from two different serotypes of Streptococcus pneumoniae [...] Read more.

The Liposomal Encapsulation of Polysaccharides (LEPS) dual antigen vaccine carrier system was assessed across two distinct polysaccharides for encapsulation efficiency, subsequent liposomal surface adornment with protein, adjuvant addition, and size and charge metrics. The polysaccharides derive from two different serotypes of Streptococcus pneumoniae and have traditionally served as the active ingredients of vaccines against pneumococcal disease. The LEPS system was designed to mimic glycoconjugate vaccines that covalently couple polysaccharides to protein carriers; however, the LEPS system uses a noncovalent co-localization mechanism through protein liposomal surface attachment. In an effort to more thoroughly characterize the LEPS system across individual vaccine components and thus support broader future utility, polysaccharides from S. pneumoniae serotypes 3 and 4 were systematically compared within the LEPS framework both pre- and post-surface protein attachment. For both polysaccharides, ≥85% encapsulation efficiency was achieved prior to protein surface attachment. Upon protein attachment with either a model protein (GFP) or a pneumococcal disease antigen (PncO), polysaccharide encapsulation was maintained at ≥61% encapsulation efficiency. Final LEPS carriers were also evaluated with and without alum as an included adjuvant, with encapsulation efficiency maintained at ≥30%, while protein surface attachment efficiency was maintained at ≥~50%. Finally, similar trends and distributions were observed across the different polysaccharides when assessed for liposomal zeta potential and size. Full article

(This article belongs to the Special Issue Biomaterial Design for Disease Applications)

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16 pages, 5566 KiB

Open AccessArticle

Dendropanax Morbifera Extract-Mediated ZnO Nanoparticles Loaded with Indole-3-Carbinol for Enhancement of Anticancer Efficacy in the A549 Human Lung Carcinoma Cell Line

by Esrat Jahan Rupa, Lakshminarayanan Arunkumar, Yaxi Han, Jong Pyo Kang, Jong Chan Ahn, Seok-Kyu Jung, Mia Kim, Jong Yun Kim, Deok-Chun Yang and Gyong Jai Lee

Materials 2020, 13(14), 3197; https://doi.org/10.3390/ma13143197 - 17 Jul 2020

Cited by 24 | Viewed by 2776

Abstract

Dendropanax morbifera is a versatile plant that has been used as a herbal medicine due to its various useful medicinal effects. To protect its active component from biological stress and increase its drug efficacy as well as drug bioavailability, nanoemulsion was prepared. Dendropanax [...] Read more.

Dendropanax morbifera is a versatile plant that has been used as a herbal medicine due to its various useful medicinal effects. To protect its active component from biological stress and increase its drug efficacy as well as drug bioavailability, nanoemulsion was prepared. Dendropanax morbifera zinc oxide nanoparticles (DM-ZnO NPs) were synthesized using the plant extract via the co-precipitation method and loaded with active indole-3-carbinol for nanoemulsion formulation using the ultrasonication process. Field emission transmission electron microscope revealed the flower shape of the Dendropanax morbifera indole-3-carbinol zinc oxide nanoemulsion (DM-ZnO-I3C-NE). In contrast, DM-ZnO NPs showed a spheroid shape that coincides agreeably with field emission electron scanning microscope. The hydrodynamic sizes by dynamic light scattering are about 65 ± 3 nm and 239.6 ± 6 nm and the crystallite sizes from X-ray diffraction are 11.52 nm and 16.07 nm for DM-ZnO NPs and DM-ZnO-I3C-NE, respectively. In vitro analysis revealed the cytotoxicity of DM-ZnO-I3C-NE against a human lung cancer cell line (A549) at 12.5 µg/mL as well as reactive oxygen species (ROS) production. The DM-ZnO-I3C-NE-induced ROS generation level was higher than that of DM-ZnO NPs and free indole-3-carbinol. The synergistic effect of DM-ZnO and indole-3-carbinol indicates DM-ZnO-I3C-NE as a potential candidate for future lung cancer drug and could be scope for functional food. Full article

(This article belongs to the Special Issue Biomaterial Design for Disease Applications)

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25 pages, 5506 KiB

Open AccessFeature PaperArticle

Sulfonic Acid Derivative-Modified SBA-15, PHTS and MCM-41 Mesoporous Silicas as Carriers for a New Antiplatelet Drug: Ticagrelor Adsorption and Release Studies

by Michał Moritz and Małgorzata Geszke-Moritz

Materials 2020, 13(13), 2913; https://doi.org/10.3390/ma13132913 - 29 Jun 2020

Cited by 12 | Viewed by 2445

Abstract

Three mesoporous, siliceous materials, i.e., SBA-15 (Santa Barbara Amorphous), PHTS (Plugged Hexagonal Templated Silica) and MCM-41 (Mobil Composition of Matter), functionalized with a sulfonic acid derivative, were successfully prepared and applied as the carriers for the poorly water-soluble drug, ticagrelor. The siliceous carriers [...] Read more.

Three mesoporous, siliceous materials, i.e., SBA-15 (Santa Barbara Amorphous), PHTS (Plugged Hexagonal Templated Silica) and MCM-41 (Mobil Composition of Matter), functionalized with a sulfonic acid derivative, were successfully prepared and applied as the carriers for the poorly water-soluble drug, ticagrelor. The siliceous carriers were characterized using nitrogen sorption analysis, X-ray diffraction (XRD), transmission electron microscopy (TEM) and elemental analysis. The adsorption studies were conducted in acetonitrile. At the highest equilibrium concentrations, the amount of ticagrelor Q_e that adsorbed onto the examined silicas was in the range of 83 to 220 mg/g, increasing in the following order: PHTS-(CH₂)₃-SO₃H < SBA-15-(CH₂)₃-SO₃H < MCM-41-(CH₂)₃-SO₃H. The equilibrium adsorption data were analyzed using the Freundlich, Jovanovich, Langmuir, Temkin, Dubinin-Radushkevich, Dubinin-Astakhov and Redlich-Peterson models. In order to find the best-fit isotherm for each model, a nonlinear fitting analysis was carried out. Based on the minimized values of the ARE function, the fit of the isotherms to the experimental points for ticagrelor adsorption onto the modified silicas can be ordered as follows: SBA-15-(CH₂)₃-SO₃H (Redlich-Peterson > Dubinin-Astakhov > Temkin), PHTS-(CH₂)₃-SO₃H (Redlich-Peterson > Temkin > Dubinin-Astakhov), MCM-41-(CH₂)₃-SO₃H (Redlich-Peterson > Dubinin-Astakhov > Langmuir). The values of adsorption energy (above 8 kJ/mol) indicate the chemical nature of ticagrelor adsorption onto propyl-sulfonic acid-modified silicas. The results of release studies indicated that at pH 4.5, modified SBA-15 and MCM-41 carriers accelerate the drug dissolution process, compared to the dissolution rate of free crystalline ticagrelor. Intriguingly, modified PHTS silica provides prolonged drug release kinetics compared to other siliceous adsorbents and to the dissolution rate of crystalline ticagrelor. A Weibull release model was employed to describe the release profiles of ticagrelor from the prepared carriers. The time necessary to dissolve 50% and 90% of ticagrelor from mesoporous adsorbents at pH 4.5 increased in the following order: SBA-15-(CH₂)₃-SO₃H < MCM-41-(CH₂)₃-SO₃H < PHTS-(CH₂)₃-SO₃H. Full article

(This article belongs to the Special Issue Biomaterial Design for Disease Applications)

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14 pages, 5307 KiB

Open AccessFeature PaperArticle

Well-Defined Diblock Poly(ethylene glycol)-b-Poly(ε-caprolactone)-Based Polymer-Drug Conjugate Micelles for pH-Responsive Delivery of Doxorubicin

by Amin Jafari, Lingyue Yan, Mohamed Alaa Mohamed, Yun Wu and Chong Cheng

Materials 2020, 13(7), 1510; https://doi.org/10.3390/ma13071510 - 26 Mar 2020

Cited by 12 | Viewed by 4521

Abstract

Nanoparticles have emerged as versatile carriers for various therapeutics and can potentially treat a wide range of diseases in an accurate and disease-specific manner. Polymeric biomaterials have gained tremendous attention over the past decades, owing to their tunable structure and properties. Aliphatic polyesters [...] Read more.

Nanoparticles have emerged as versatile carriers for various therapeutics and can potentially treat a wide range of diseases in an accurate and disease-specific manner. Polymeric biomaterials have gained tremendous attention over the past decades, owing to their tunable structure and properties. Aliphatic polyesters have appealing attributes, including biodegradability, non-toxicity, and the ability to incorporate functional groups within the polymer backbone. Such distinctive properties have rendered them as a class of highly promising biomaterials for various biomedical applications. In this article, well-defined alkyne-functionalized poly(ethylene glycol)-b-poly(ε-caprolactone) (PEG-b-PCL) diblock copolymer was synthesized and studied for pH-responsive delivery of doxorubicin (DOX). The alkyne-functionalized PEG-b-PCL diblock copolymer was prepared by the synthesis of an alkyne-functionalized ε-caprolactone (CL), followed by ring-opening polymerization (ROP) using PEG as the macroinitiator. The alkyne functionalities of PEG-b-PCL were modified through copper(I)-catalyzed alkyne-azide cycloaddition (CuAAC) click reaction to graft aldehyde (ALD) groups and obtain PEG-b-PCL-g-ALD. Subsequently, DOX was conjugated on PEG-b-PCL-g-ALD through the Schiff base reaction. The resulting PEG-b-PCL-g-DOX polymer-drug conjugate (PDC) self-assembled into a nano-sized micellar structure with facilitated DOX release in acidic pH due to the pH-responsive linkage. The nanostructures of PDC micelles were characterized using transmission electron microscopy (TEM) and dynamic light scattering (DLS). In vitro studies of the PDC micelles, revealed their improved anticancer efficiency towards MCF-7 cells as compared to free DOX. Full article

(This article belongs to the Special Issue Biomaterial Design for Disease Applications)

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17 pages, 5526 KiB

Open AccessArticle

PEGylated Amine-Functionalized Poly(ε-caprolactone) for the Delivery of Plasmid DNA

by Amin Jafari, Nika Rajabian, Guojian Zhang, Mohamed Alaa Mohamed, Pedro Lei, Stelios T. Andreadis, Blaine A. Pfeifer and Chong Cheng

Materials 2020, 13(4), 898; https://doi.org/10.3390/ma13040898 - 18 Feb 2020

Cited by 8 | Viewed by 5178

Abstract

As a promising strategy for the treatment of various diseases, gene therapy has attracted increasing attention over the past decade. Among various gene delivery approaches, non-viral vectors made of synthetic biomaterials have shown significant potential. Due to their synthetic nature, non-viral vectors can [...] Read more.

As a promising strategy for the treatment of various diseases, gene therapy has attracted increasing attention over the past decade. Among various gene delivery approaches, non-viral vectors made of synthetic biomaterials have shown significant potential. Due to their synthetic nature, non-viral vectors can have tunable structures and properties by using various building units. In particular, they can offer advantages over viral vectors with respect to biosafety and cytotoxicity. In this study, a well-defined poly(ethylene glycol)-block-poly(α-(propylthio-N,N-diethylethanamine hydrochloride)-ε-caprolactone) diblock polymer (PEG-b-CPCL) with one poly(ethylene glycol) (PEG) block and one tertiary amine-functionalized cationic poly(ε-caprolactone) (CPCL) block, as a novel non-viral vector in the delivery of plasmid DNA (pDNA), was synthesized and studied. Despite having a degradable polymeric structure, the polymer showed remarkable hydrolytic stability over multiple weeks. The optimal ratio of the polymer to pDNA for nanocomplex formation, pDNA release from the nanocomplex with the presence of heparin, and serum stability of the nanocomplex were probed through gel electrophoresis. Nanostructure of the nanocomplexes was characterized by DLS and TEM imaging. Relative to CPCL homopolymers, PEG-b-CPCL led to better solubility over a wide range of pH. Overall, this work demonstrates that PEG-b-CPCL possesses a range of valuable properties as a promising synthetic vector for pDNA delivery. Full article

(This article belongs to the Special Issue Biomaterial Design for Disease Applications)

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12 pages, 2869 KiB

Open AccessArticle

The Radiosensitizing Effect of Zinc Oxide Nanoparticles in Sub-Cytotoxic Dosing Is Associated with Oxidative Stress In Vitro

by Till Jasper Meyer, Agmal Scherzad, Helena Moratin, Thomas Eckert Gehrke, Julian Killisperger, Rudolf Hagen, Gisela Wohlleben, Bülent Polat, Sofia Dembski, Norbert Kleinsasser and Stephan Hackenberg

Materials 2019, 12(24), 4062; https://doi.org/10.3390/ma12244062 - 5 Dec 2019

Cited by 8 | Viewed by 2738

Abstract

Radioresistance is an important cause of head and neck cancer therapy failure. Zinc oxide nanoparticles (ZnO-NP) mediate tumor-selective toxic effects. The aim of this study was to evaluate the potential for radiosensitization of ZnO-NP. The dose-dependent cytotoxicity of ZnO-NP_{20 nm} and ZnO-NP [...] Read more.

Radioresistance is an important cause of head and neck cancer therapy failure. Zinc oxide nanoparticles (ZnO-NP) mediate tumor-selective toxic effects. The aim of this study was to evaluate the potential for radiosensitization of ZnO-NP. The dose-dependent cytotoxicity of ZnO-NP_{20 nm} and ZnO-NP_{100 nm} was investigated in FaDu and primary fibroblasts (FB) by an MTT assay. The clonogenic survival assay was used to evaluate the effects of ZnO-NP alone and in combination with irradiation on FB and FaDu. A formamidopyrimidine-DNA glycosylase (FPG)-modified single-cell microgel electrophoresis (comet) assay was applied to detect oxidative DNA damage in FB as a function of ZnO-NP and irradiation exposure. A significantly increased cytotoxicity after FaDu exposure to ZnO-NP_{20 nm} or ZnO-NP_{100 nm} was observed in a concentration of 10 µg/mL or 1 µg/mL respectively in 30 µg/mL of ZnO-NP_{20 nm} or 20 µg/mL of ZnO-NP_{100 nm} in FB. The addition of 1, 5, or 10 µg/mL ZnO-NP_{20 nm} or ZnO-NP_{100 nm} significantly reduced the clonogenic survival of FaDu after irradiation. The sub-cytotoxic dosage of ZnO-NP_{100 nm} increased the oxidative DNA damage compared to the irradiated control. This effect was not significant for ZnO-NP_{20 nm}. ZnO-NP showed radiosensitizing properties in the sub-cytotoxic dosage. At least for the ZnO-NP_{100 nm}, an increased level of oxidative stress is a possible mechanism of the radiosensitizing effect. Full article

(This article belongs to the Special Issue Biomaterial Design for Disease Applications)

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9 pages, 3933 KiB

Open AccessArticle

Novel Eco-Synthesis of PD Silver Nanoparticles: Characterization, Assessment of Its Antimicrobial and Cytotoxicity Properties

by Manal A. Awad, Manal M. Alkhulaifi, Noura S. Aldosari, Shaykha Alzahly and Ali Aldalbahi

Materials 2019, 12(23), 3890; https://doi.org/10.3390/ma12233890 - 25 Nov 2019

Cited by 11 | Viewed by 3469

Abstract

Nanomedicine is growing due to the development of new medical diagnostic tools and new nanostructure-based therapies that exert direct biological action or function as pharmacological carriers. Nanoparticles (NPs) synthesis provides an eco-friendly approach for different applications. Among NPs, silver NPs (AgNPs) are gaining [...] Read more.

Nanomedicine is growing due to the development of new medical diagnostic tools and new nanostructure-based therapies that exert direct biological action or function as pharmacological carriers. Nanoparticles (NPs) synthesis provides an eco-friendly approach for different applications. Among NPs, silver NPs (AgNPs) are gaining considerable research interest due to their broad range of activity and their usability in the medical and biotechnology fields. In this study, a new AgNP synthesis method was developed using an aqueous pigeon dropping (PD) extract in silver nitrate (AgNO₃). The rapid of AgNPs yield was detected visually. Analysis of UV-vis spectroscopy, energy-dispersive X-ray spectroscopy (EDX), dynamic light scattering (DLS) and electron microscopy (TEM) transmission showed a spherical or near spherical shape of AgNPs with mean size of 135 nm. AgNPs antimicrobial activities (anti-bacterial and anti-fungal) were determined using agar well diffusion method. These NPs further screened for anticancer activity in vitro using A-549 and MCF-7 cell lines. The results showed that the inhibition zone for the obtained PD AgNPs versus Escherichia coli, Pseudomonas aeruginosa, Staphylococcus aureus, and Bacillus were 26, 18, 17 and 15 mm, respectively. PD AgNPs showed the highest antifungal effect against Aspergillus flavus and the lowest effect against Penicillium griseofulvum. In vitro anti-cancer activities showed that the inhibitory concentration of 50% (IC₅₀) of AgNPs was 10.3 ± 1.15 and 12.19 ± 0.75 µg mL⁻¹ against A-549 and MCF-7 cancer cell lines, respectively. Full article

(This article belongs to the Special Issue Biomaterial Design for Disease Applications)

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13 pages, 2309 KiB

Open AccessArticle

Randomized Controlled Clinical Trial of Nanostructured Carbonated Hydroxyapatite for Alveolar Bone Repair

by Rodrigo F. B. Resende, Suelen C. Sartoretto, Marcelo J. Uzeda, Adriana T. N. N. Alves, José A. Calasans-Maia, Alexandre M. Rossi, José Mauro Granjeiro and Mônica D. Calasans-Maia

Materials 2019, 12(22), 3645; https://doi.org/10.3390/ma12223645 - 6 Nov 2019

Cited by 18 | Viewed by 2827

Abstract

The properties of the biodegradation of bone substitutes in the dental socket after extraction is one of the goals of regenerative medicine. This double-blind, randomized, controlled clinical trial aimed to compare the effects of a new bioabsorbable nanostructured carbonated hydroxyapatite (CHA) with a [...] Read more.

The properties of the biodegradation of bone substitutes in the dental socket after extraction is one of the goals of regenerative medicine. This double-blind, randomized, controlled clinical trial aimed to compare the effects of a new bioabsorbable nanostructured carbonated hydroxyapatite (CHA) with a commercially available bovine xenograft (Bio-Oss^®) and clot (control group) in alveolar preservation. Thirty participants who required tooth extraction and implant placement were enrolled in this study. After 90 days, a sample of the grafted area was obtained for histological and histomorphometric evaluation and an implant was installed at the site. All surgical procedures were successfully carried out without complications and none of the patients were excluded. The samples revealed a statistically significant increase of new bone formation (NFB) in the CHA group compared with Bio-Oss^® after 90 days from surgery (p < 0.05). However, the clot group presented no differences of NFB compared to CHA and Bio-Oss^®. The CHA group presented less amount of reminiscent biomaterial compared to Bio-Oss^®. Both biomaterials were considered osteoconductors, easy to handle, biocompatible, and suitable for alveolar filling. Nanostructured carbonated hydroxyapatite spheres promoted a higher biodegradation rate and is a promising biomaterial for alveolar socket preservation before implant treatment. Full article

(This article belongs to the Special Issue Biomaterial Design for Disease Applications)

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10 pages, 2387 KiB

Open AccessArticle

Design Variation of a Dual-Antigen Liposomal Vaccine Carrier System

by Roozbeh Nayerhoda, Andrew Hill, Marie Beitelshees, Charles Jones and Blaine Pfeifer

Materials 2019, 12(17), 2809; https://doi.org/10.3390/ma12172809 - 1 Sep 2019

Cited by 2 | Viewed by 3423

Abstract

The enclosed work focuses on the construction variables associated with a dual-antigen liposomal carrier, delivering encapsulated polysaccharides and surface-localized proteins, which served as a vaccine delivery device effective against pneumococcal disease. Here, the goal was to better characterize and compare the carrier across [...] Read more.

The enclosed work focuses on the construction variables associated with a dual-antigen liposomal carrier, delivering encapsulated polysaccharides and surface-localized proteins, which served as a vaccine delivery device effective against pneumococcal disease. Here, the goal was to better characterize and compare the carrier across a range of formulation steps and assessment metrics. Specifically, the vaccine carrier was subjected to new methods of liposomal formation, including alterations to the base components used for subsequent macromolecule encapsulation and surface attachment, with characterization spanning polysaccharide encapsulation, liposomal size and charge, and surface protein localization. Results demonstrate variations across the liposomal constructs comprised two means of surface-localizing proteins (either via metal or biological affinity). In general, final liposomal constructs demonstrated a size and zeta potential range of approximately 50 to 600 nm and −4 to −41 mV, respectively, while demonstrating at least 60% polysaccharide encapsulation efficiency and 60% protein surface localization for top-performing liposomal carrier constructs. The results, thus, indicate that multiple formulations could serve in support of vaccination studies, and that the selection of a suitable final delivery system would be dictated by preferences or requirements linked to target antigens and/or regulatory demands. Full article

(This article belongs to the Special Issue Biomaterial Design for Disease Applications)

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10 pages, 2126 KiB

Open AccessArticle

pH-Sensitive Ratiometric Fluorescent Probe for Evaluation of Tumor Treatments

by Peisen Zhang, Junli Meng, Yingying Li, Zihua Wang and Yi Hou

Materials 2019, 12(10), 1632; https://doi.org/10.3390/ma12101632 - 18 May 2019

Cited by 17 | Viewed by 3571

Abstract

Determining therapeutic efficacy is critical for tumor precision theranostics. In order to monitor the efficacy of anti-cancer drugs (e.g., Paclitaxel), a pH-sensitive ratiometric fluorescent imaging probe was constructed. The pH-sensitive ratiometric fluorescent dye ANNA was covalently coupled to the N-terminal of the cell-penetrating [...] Read more.

Determining therapeutic efficacy is critical for tumor precision theranostics. In order to monitor the efficacy of anti-cancer drugs (e.g., Paclitaxel), a pH-sensitive ratiometric fluorescent imaging probe was constructed. The pH-sensitive ratiometric fluorescent dye ANNA was covalently coupled to the N-terminal of the cell-penetrating TAT peptide through an amidation reaction (TAT-ANNA). The in vitro cellular experiments determined that the TAT-ANNA probe could penetrate the cell membrane and image the intracellular pH in real time. The in vivo experiments were then carried out, and the ratiometric pH response to the state of the tumor was recorded immediately after medication. The TAT-ANNA probe was successfully used to monitor the pharmacodynamics of anti-cancer drugs in vivo. Full article

(This article belongs to the Special Issue Biomaterial Design for Disease Applications)

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10 pages, 1206 KiB

Open AccessArticle

Potential of Chemical and Physical Enhancers for Transungual Delivery of Amorolfine Hydrochloride

by Indrė Šveikauskaitė, Alius Pockevičius and Vitalis Briedis

Materials 2019, 12(7), 1028; https://doi.org/10.3390/ma12071028 - 28 Mar 2019

Cited by 15 | Viewed by 3574

Abstract

Topical monotherapy of nail infection is limited by poor drug permeability into the human nail plate. Numerous substances and methods are applied to improve the antifungal agent delivery across the nail plate. This work aimed to evaluate the effect of chemical and physical [...] Read more.

Topical monotherapy of nail infection is limited by poor drug permeability into the human nail plate. Numerous substances and methods are applied to improve the antifungal agent delivery across the nail plate. This work aimed to evaluate the effect of chemical and physical enhancers on the accumulation and permeation of amorolfine hydrochloride through human nail clippings. Polymeric nail lacquers with Eudragit E100 were developed as a potentially suitable delivery system for amorolfine hydrochloride. Incorporating thioglycolic acid and urea into formulations provided increased accumulation of antifungal agent in nail layers of up to 100% and 57%, respectively. Structural changes of nail barrier, induced by fractional CO₂ laser, were visualized by microscopy. The permeation of amorolfine hydrochloride through the nail increased twofold when thioglycolic acid-containing formulation was applied and the nail was pretreated with a fractional CO₂ laser. The results suggest that this novel combination of enhancers has the potential to be an effective option for topical drug delivery through the nail, and increased the efficacy of treatment. Full article

(This article belongs to the Special Issue Biomaterial Design for Disease Applications)

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