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Polyphenols delivery by polymeric materials: challenges in cancer treatment
Nanotechnology can offer different solutions for enhancing the therapeutic efficiency of polyphenols, a class of natural products widely explored for a potential applicability for the treatment of different diseases including cancer. While possessing interesting anticancer properties, polyphenols suffer from low stability and unfavorable pharmacokinetics, and thus suitable carriers are required when planning a therapeutic protocol. In the present review, an overview of the different strategies based on polymeric materials is presented, with the aim to highlight the strengths and the weaknesses of each approach and offer a platform of ideas for researchers working in the field.
Magnetic Graphene Oxide Nanocarrier for Targeted Delivery of Cisplatin : A Perspective for Glioblastoma Treatment
Selective vectorization of Cisplatin (CisPt) to Glioblastoma U87 cells was exploited by the fabrication of a hybrid nanocarrier composed of magnetic γ-Fe2 O3 nanoparticles and nanographene oxide (NGO). The magnetic component, obtained by annealing magnetite Fe3 O4 and characterized by XRD measurements, was combined with NGO sheets prepared via a modified Hummer’s method. The morphological and thermogravimetric analysis proved the effective binding of γ-Fe2 O3 nanoparticles onto NGO layers. The magnetization measured under magnetic fields up to 7 Tesla at room temperature revealed superparamagnetic-like behavior with a maximum value of MS = 15 emu/g and coercivity HC ≈ 0 Oe within experimental error. The nanohybrid was found to possess high affinity towards CisPt, and a rather slow fractional release profile of 80% after 250 h. Negligible toxicity was observed for empty nanoparticles, while the retainment of CisPt anticancer activity upon loading into the carrier was observed, together with the possibility to spatially control the drug delivery at a target site. © 2019 by the authors. Licensee MDPI, Basel, Switzerland.
Carbon nanotubes hybrid hydrogels in drug delivery: A perspective review
The use of biologics, polymers, silicon materials, carbon materials, and metals has been proposed for the preparation of innovative drug delivery devices. One of the most promising materials in this field are the carbon-nanotubes composites and hybrid materials coupling the advantages of polymers (biocompatibility and biodegradability) with those of carbon nanotubes (cellular uptake, stability, electromagnatic, and magnetic behavior). The applicability of polymer-carbon nanotubes composites in drug delivery, with particular attention to the controlled release by composites hydrogel, is being extensively investigated in the present review.
Carbon Nanotubes Hybrid Hydrogels for Environmental Remediation: Evaluation of Adsorption Efficiency under Electric Field
The performance of Carbon Nanotubes hybrid hydrogels for environmental remediation was investigated using Methylene Blue (MB), Rhodamine B (RD), and Bengal Rose (BR) as model contaminating dyes. An acrylate hydrogel network with incorporated CNT was synthesized by photo-polymerization without any preliminary derivatization of CNT surface. Thermodynamics, isothermal and kinetic studies showed favorable sorption processes with the application of an external 12 V electric field found to be able to influence the amount of adsorbed dyes: stronger interactions with cationic MB molecules (qexp and q12exp of 19.72 and 33.45 mg g−1, respectively) and reduced affinity for anionic RD (qexp and q12exp of 28.93 and 13.06 mg g−1, respectively) and neutral BR (qexp and q12exp of 36.75 and 15.85 mg g−1, respectively) molecules were recorded. The influence of pH variation on dyes adsorption was finally highlighted by reusability studies, with the negligible variation of adsorption capacity after five repeated sorption cycles claiming for the suitability of the proposed systems as effective sorbent for wastewater treatment.
Functionalized carbon nanotubes as transporters for antisense oligodeoxynucleotides
The use of DNA-based therapeutics requires efficient delivery systems to transport the DNA to their place of action within the cell. To accomplish this, we investigated multiwalled carbon nanotubes (pristine MWCNT, p-MWCNT) functionalized with hydroxyl groups via 1,3-dipolar cycloaddition. In this way, we have obtained MWCNT-f-OH with improved stability in aqueous dispersions which is an advantageous property for their use in cellular environments. Afterwards, a carrier strand oligodeoxynucleotide (CS-ODN) was adsorbed to MWCNT-f-OH followed by hybridization with a therapeutic antisense oligodeoxynucleotide (AS-ODN). The amount of adsorbed CS-ODN, as well as the complementary AS-ODN and a non-complementary oligodeoxynucleotide (NS-ODN) as reference, was directly measured by radionuclide labeling of ODNs. We show that subsequent release of AS-ODNs and NS-ODNs was possible for MWCNT-f-OH above the melting temperature of AS-ODNs at 80 °C and under physiological conditions at different pH values at 37 °C. We also show a very low influence of p-MWCNT and MWCNT-f-OH on the cell viability of the bladder carcinoma (BCa) cell line EJ28 and that both MWCNT types were internalized by EJ28. Therefore, MWCNT-f-OH represents a promising carrier able to transport and release AS-ODNs inside cells.
Recent advances in the synthesis and biomedical applications of nanocomposite hydrogels
Hydrogels sensitive to electric current are usually made of polyelectrolytes and undergo erosion, swelling, de-swelling or bending in the presence of an applied electric field. The electrical conductivity of many polymeric materials used for the fabrication of biomedical devices is not high enough to achieve an effective modulation of the functional properties, and thus, the incorporation of conducting materials (e.g., carbon nanotubes and nanographene oxide) was proposed as a valuable approach to overcome this limitation. By coupling the biological and chemical features of both natural and synthetic polymers with the favourable properties of carbon nanostructures (e.g., cellular uptake, electromagnetic and magnetic behaviour), it is possible to produce highly versatile and effective nanocomposite materials. In the present review, the recent advances in the synthesis and biomedical applications of electro-responsive nanocomposite hydrogels are discussed.
Curcumin and Graphene Oxide Incorporated into Alginate Hydrogels as Versatile Devices for the Local Treatment of Squamous Cell Carcinoma
With the aim of preparing hybrid hydrogels suitable for use as patches for the local treatment of squamous cell carcinoma (SCC)-affected areas, curcumin (CUR) was loaded onto graphene oxide (GO) nanosheets, which were then blended into an alginate hydrogel that was crosslinked by means of calcium ions. The homogeneous incorporation of GO within the polymer network, which was confirmed through morphological investigations, improved the stability of the hybrid system compared to blank hydrogels. The weight loss in the 100–170 °C temperature range was reduced from 30% to 20%, and the degradation of alginate chains shifted to higher temperatures. Moreover, GO enhanced the stability in water media by counteracting the de-crosslinking process of the polymer network. Cell viability assays showed that the loading of CUR (2.5% and 5% by weight) was able to reduce the intrinsic toxicity of GO towards healthy cells, while higher amounts were ineffective due to the antioxidant/prooxidant paradox. Interestingly, the CUR-loaded systems were found to possess a strong cytotoxic effect in SCC cancer cells, and the sustained CUR release (~50% after 96 h) allowed long-term anticancer efficiency to be hypothesized.
Release of Bioactive Molecules from Graphene Oxide-Alginate Hybrid Hydrogels: Effect of Crosslinking Method
To investigate the influence of crosslinking methods on the releasing performance of hybrid hydrogels, we synthesized two systems consisting of Graphene oxide (GO) as a functional element and alginate as polymer counterpart by means of ionic gelation (physical method, 𝐻𝑃𝐴−𝐺𝑂) and radical polymerization (chemical method, 𝐻𝐶𝐴−𝐺𝑂). Formulations were optimized to maximize the GO content (2.0 and 1.15% for 𝐻𝑃𝐴−𝐺𝑂 and 𝐻𝐶𝐴−𝐺𝑂, respectively) and Curcumin (CUR) was loaded as a model drug at 2.5, 5.0, and 7.5% (by weight). The physico-chemical characterization confirmed the homogeneous incorporation of GO within the polymer network and the enhanced thermal stability of hybrid vs. blank hydrogels. The determination of swelling profiles showed a higher swelling degree for 𝐻𝐶𝐴−𝐺𝑂 and a marked pH responsivity due to the COOH functionalities. Moreover, the application of external voltages modified the water affinity of 𝐻𝐶𝐴−𝐺𝑂, while they accelerated the degradation of 𝐻𝑃𝐴−𝐺𝑂 due to the disruption of the crosslinking points and the partial dissolution of alginate. The evaluation of release profiles, extensively analysed by the application of semi-empirical mathematical models, showed a sustained release from hybrid hydrogels, and the possibility to modulate the releasing amount and rate by electro-stimulation of 𝐻𝐶𝐴−𝐺𝑂.
Facile one-pot hydrothermal synthesis of a zinc oxide/curcumin nanocomposite with enhanced toxic activity against breast cancer cells
Zinc oxide/Curcumin (Zn(CUR)O) nanocomposites were prepared via hydrothermal treatment of Zn(NO3)2 in the presence of hexamethylenetetramine as a stabilizing agent and CUR as a bioactive element. Three ZnO : CUR ratios were investigated, namely 57 : 43 (Zn(CUR)O-A), 60 : 40 (Zn(CUR)O-B) and 81 : 19 (Zn(CUR)O-C), as assessed by thermogravimetric analyses, with an average hydrodynamic diameter of nanoaggregates in the range of 223 to 361 nm. The interaction of CUR with ZnO via hydroxyl and ketoenol groups (as proved by X-ray photoelectron spectroscopy analyses) was found to significantly modify the key properties of ZnO nanoparticles with the obtainment of a bilobed shape (as shown by scanning electron microscopy), and influenced the growth process of the composite nanoparticles as indicated by the varying particle sizes determined by powder X-ray diffraction. The efficacy of Zn(CUR)O as anticancer agents was evaluated on MCF-7 and MDA-MB-231 cancer cells, obtaining a synergistic activity with a cell viability depending on the CUR amount within the nanocomposite. Finally, the determination of reactive oxygen species production in the presence of Zn(CUR)O was used as a preliminary evaluation of the mechanism of action of the nanocomposites.