Modification of Polyhedral Oligomeric Silsesquioxanes (POSS) Molecules by Ruthenium Catalyzed Cross Metathesis.
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ABSTRACT:
SUBMITTER: Czaban-Jozwiak J
PROVIDER: S-EPMC6099925 | biostudies-literature |
REPOSITORIES: biostudies-literature
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Project description:In this study, a tetrafunctional epoxy resin was loaded with 5 wt% of three different types of polyhedral oligomeric silsesquioxane (POSS) compounds, namely, DodecaPhenyl POSS (DPHPOSS), Epoxycyclohexyl POSS (ECPOSS), Glycidyl POSS (GPOSS), and 0.5 wt% of multi-walled carbon nanotubes (CNTs) in order to formulate multifunctional structural nanocomposites tailored for aeronautic and aerospace applications. This work aims to demonstrate how the skillful combination of desired properties, such as good electrical, flame-retardant, mechanical, and thermal properties, is obtainable thanks to the advantages connected with nanoscale incorporations of nanosized CNTs with POSS. The special hydrogen bonding-based intermolecular interactions between the nanofillers have proved to be strategic in imparting multifunctionality to the nanohybrids. All multifunctional formulations are characterized by a Tg centered at values close to 260 °C, fully satisfying structural requirements. Infrared spectroscopy and thermal analysis confirm the presence of a cross-linked structure characterized by a high curing degree of up to 94% and high thermal stability. Tunneling atomic force microscopy (TUNA) allows to detect the map of the electrical pathways at the nanoscale of the multifunctional samples, highlighting a good dispersion of the carbon nanotubes within the epoxy resin. The combined action of POSS with CNTs has allowed to obtain the highest values of self-healing efficiency if compared to those measured for samples containing only POSS in the absence of CNTs.
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Project description:Hydrophobic coatings have considerable potential applications in many fields. Ease of operation and high durability are essential for practical use. Fast curing and being solvent-free are a plus, and if they possess certain characteristics (antigraffiti, good adhesion, high hardness, heat resistance, wide range of applicability, etc.) at the same time, it is a dream solution. Herein, a facile one-step approach with the above features was reported for a UV curable robust hydrophobic coating based on Epoxy Polyhedral Oligomeric Silsesquioxanes (EP-POSSs). The structure and surface morphology of these EP-POSSs and their derivatives were systematically studied. Because of the core-in-cage structure which was constructed by repeating units of R-Si(O1/2)3 and the strong covalent bonds of Si-C and Si-O, the coatings displayed high pencil hardness (6-8H), high thermal stability with initial decomposition temperature around 350-400 °C, and a high water contact angle (up to 108.06°) even after outdoor exposure for a month. These POSSs and their derivatives are expected to find uses in various applications such as stain resistance, self-cleaning, scratch resistance, and cigarette moxibustion resistance of wood furniture, kitchenware, and medical and industrial appliances.
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Project description:Anthracyclines belong to the anticancer drugs that are widely used in chemotherapy. However, due to their systemic toxicity they also exert dangerous side effects associated mainly with cardiovascular risks. The pathway that is currently often developed is their chemical and physical modification via formation of conjugated or complexed prodrug systems with a variety of nanocarriers that can selectively release the active species in cancer cells. In this study, six new nanoconjugates were synthesized with the use of polyhedral oligosilsesquioxanes [POSS(OH)32] as nanocarriers of the anticancer drugs anthracyclines-doxorubicin (DOX) and daunorubicin (DAU). These prodrug conjugates are also equipped with poly(ethylene glycol) (PEG) moieties of different structure and molecular weight. Water-soluble POSS, succinic anhydride modified (SAMDOX and SAMDAU) with carboxylic function, and PEGs (PEG1, PEG2 and PEGB3) were used for the synthesis. New nanoconjugates were formed via ester bonds and their structure was confirmed by NMR spectroscopy (1H-NMR, 13C-NMR, 1H-13C HSQC, DOSY and 1H-1H COSY), FTIR and DLS. Drug release rate was evaluated using UV-Vis spectroscopy at pH of 5.5. Release profiles of anthracyclines from conjugates 4-9 point to a range of 10 to 75% (after 42 h). Additionally, model NMR tests as well as diffusion ordered spectroscopy (DOSY) confirmed formation of the relevant prodrugs. The POSS-anthracycline conjugates exhibited prolonged active drug release time that can lead to the possibility of lowering administered doses and thus giving them high potential in chemotherapy. Drug release from conjugate 7 after 42 h was approx. 10%, 33% for conjugate 4, 47% for conjugate 5, 6, 8 and 75% for conjugate 9.
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Project description:A single-step molding process utilizing free-radical cross-linking reaction of vinyl POSS in microliter-sized dimensions leads to hierarchically-structured, mechanically robust, porous hybrid structures. Functional variants show excellent performance in Suzuki-type coupling reactions. Due to their small volume, long-term operational robustness, and potential chemical diversity, these materials are promising candidates for catalyst screening applications.
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Project description:In this study, we report UV-MALDI-TOF MS evidence of a fullerene-like silsesquioxane, a high-symmetry polyhedral oligomeric silsesquioxane (POSS or SSO) formulated as R60-Si60O90 or T60 (T = RSiO1.5). The T60 preparation can be performed using a normal hydrolytic condensation of [(3-methacryloxy)propyl]trimethoxysilane (MPMS) as an example. Theoretically, four 3sp³ hybrid orbitals (each containing an unpaired electron) of a Si atom are generated before the bond formation. Then it bonds to another four atom electrons using the four generated hybrid orbitals which produced a stable configuration. This fullerene-like silsesquioxane should exhibit much more functionality, activity and selectivity and is easier to assemble than the double bonds in a fullerene.
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Project description:Silicon quantum dots (SiQDs) and carbon quantum dots (CQDs) are renowned for their outstanding applications in fluorescence imaging and biosensing. However, their small size poses significant challenges in terms of preparation, collection, and purification. Polyhedral oligomeric silsesquioxanes (POSS), an organic-inorganic nanohybrid with a cage-like structure, has recently attracted considerable attention due to its excellent biocompatibility. In this research, we utilize the encapsulating properties of POSS to improve the optical property of SiQDs/CQDs through an in situ synthesis strategy, resulting in the production of blue-emitting POSS-SiQDs, green-emitting POSS-G-CNDs, and red-emitting POSS-R-CNDs. By examining their structural and optical characteristics, it is found that these hybrid materials exhibit excellent luminescent properties, biocompatibility and cell membrane permeability. This facilitates multicolor intracellular imaging and underscores their successful application in biological imaging. Our study presents a novel approach to synthesize POSS-QDs composite nanomaterials with new perspectives in biological imaging and medical diagnostics.
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Project description:Suitable polymers for the homogeneous formulation of drug/polymer mixtures should be selected to correct the structural and physicochemical nature with a rapid dissolution rate. This study aimed to evaluate a copolymer prepared by the radical polymerization of 2-methacryloyloxyethyl phosphorylcholine (MPC) and a polyhedral oligomeric silsesquioxane (POSS) methacrylate bearing an ethyl (C₂H₅) group (MPC-ran-C₂H₅-POSS) as a carrier for the solid formulation of paclitaxel (PTX). A single-phase homogeneous formulation of PTX with the mixture of the MPC-ran-C₂H₅-POSS and polyvinylpyrrolidone (PVP) was prepared by a solvent method. The formulation of MPC-ran-C₂H₅-POSS/PVP/PTX enhanced the dissolution rate and the dissolved amount (approximately 90% within 40 min) without precipitation. The X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FT-IR) and differential scanning calorimetry (DSC) analysis confirmed the presence of PTX as an amorphous state. The amphiphilic nature of the MPC-ran-C₂H₅-POSS contributed to enhancing the aqueous solubility of PTX. The new formulation is applicable for solid dispersion technique via the supersaturation of PTX in an aqueous media.
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Project description:Electrochromic devices (ECDs) exhibit reversible optical changes under applied electrical stimuli. Transparent conducting electrodes (TCOs), generally constructed with indium tin oxide (ITO), are a vital component determining transparency and switching behaviors. ITO specifications for TCO materials have not drawn much attention despite the critical role of these materials. Herein we investigate the influence of ITO electrodes in achieving high-performance ECDs containing viologen-functionalized polyhedral oligomeric silsesquioxane (POSS-viologen). Indeed, ITO electrodes exert significant effects on the electrochromic characteristics. A high ITO thickness shows superior color-switching with high optical density and coloration efficiency levels. Enhanced electrical conductivity facilitates diffusion behaviors, an outcome beneficial for electrochromic switching. The surface-charge capacity ratio values are measured and found to be close to one, indicating that no residual current remains, and the prepared devices provide good reversibility during the coloring and bleaching process. Furthermore, with an increase in the ITO thickness, the current required for the coloring and bleaching processes decreases, and the power consumption needed for the operation of the device becomes low. The superiority of POSS-viologen should also be noted, especially when compared to normal viologens, in terms of the electrochromic properties and long-term operational stability. These results demonstrate the critical role of electrical conductivity in ITO electrodes, providing a valuable guideline for TCO specifications for ECD fabrication using viologen derivatives.
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Project description:In this study, two different types of hybrid porous organic polymers (POPs), polyhedral oligomeric silsesquioxane tetraphenylpyrazine (POSS-TPP) and tetraphenylethene (POSS-TPE), were successfully synthesized through the Friedel-Crafts polymerization of tetraphenylpyrazine (TPP) and tetraphenylethene (TPE), respectively, with octavinylsilsesquioxane (OVS) as node building blocks, in the presence of anhydrous FeCl3 as a catalyst and 1,2-dichloroethane at 60 °C. Based on N2 adsorption and thermogravimetric analyses, the resulting hybrid porous materials displayed high surface areas (270 m2/g for POSS-TPP and 741 m2/g for POSS-TPE) and outstanding thermal stabilities. Furthermore, as-prepared POSS-TPP exhibited a high carbon dioxide capacity (1.63 mmol/g at 298 K and 2.88 mmol/g at 273 K) with an excellent high adsorption capacity for iodine, reaching up to 363 mg/g, compared with the POSS-TPE (309 mg/g).
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Project description:Olefin metathesis is now one of the most efficient ways to create new carbon-carbon bonds. While most efforts focused on the development of ever-more efficient catalysts, a particular attention has recently been devoted to developing latent metathesis catalysts, inactive species that need an external stimulus to become active. This furnishes an increased control over the reaction which is crucial for applications in materials science. Here, we report our work on the development of a new system to achieve visible-light-controlled metathesis by merging olefin metathesis and photoredox catalysis. The combination of a ruthenium metathesis catalyst bearing two N-heterocyclic carbenes with an oxidizing pyrylium photocatalyst affords excellent temporal and spatial resolution using only visible light as stimulus. Applications of this system in synthesis, as well as in polymer patterning and photolithography with spatially resolved ring-opening metathesis polymerization, are described.
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