We have simulated the melt of poly(carbosilane) dendrimers using atomistic models and have reproduced the effect predicted by the analytical theory; i.e., orientational autocorrelation functions of a segment from the same layer (numbered from periphery) are practically identical and do not depend on dendrimer size. The frequency dependences of the dielectric and NMR relaxation were obtained and studied in detail. The main contribution to the maxima of these dependences is given by the pulsation process. It leads to a shift of the maxima to low frequencies for the core segment in comparison with the maxima for peripheral segments. The contribution of local reorientation can also be significant, and in some cases this contribution manifests as an additional maximum. The nontrivial scaling laws in the frequency dependences of dielectric permittivity and NMR relaxation rate averaged over all layers of a dendrimer macromolecule are found. A similar scaling law is observed in the experiments on NMR relaxation but is not described by the analytical theory.
Novel supported membranes based on polyvinyl alcohol (PVA) were developed using two strategies: first, by the modification of the PVA network, via so-called bulk modification, with the formation of the selective layer accomplished through the introduction of fullerenol and/or poly(allylamine hydrochloride), and second, by the functionalization of the surface with successive depositions of multilayered films of polyelectrolytes, such as poly(allylamine hydrochloride) and poly(sodium 4-styrenesulfonate) on the PVA surface. The membrane surface modifications were characterized by scanning electron microscopy and contact angle measurements. The modified PVA membranes were examined for their dehydration transport properties by the pervaporation of isopropyl alcohol-water (80/20% w/w), which was chosen as a model mixture. Compared with the pristine PVA membrane, the main improvement was a marked increase in permeance. It was found that the surface modifications mainly gave rise to a higher global flux but with a strong reduction in selectivity. Only the combination of both bulk and surface modifications with PEL could significantly increase the flux with a high water content in the permeate (over 98%). Lastly, it should be noted that this study developed a green procedure to prepare innovative membrane layers for dehydration, making use of only water as a working medium.
The so-called Graftfast reaction in water and at room temperature (RT) was applied to graft polyethylene glycol (PEG) at the surface of the microporous zeolitic imidazolate framework ZIF-8 nanoparticles (NPs) using acrylPEG of different chain lengths (480 Da and 5 kDa). In comparison to non-modified ZIF-8 NPs, both chemical and colloidal stabilities of PEGylated ZIF-8 NPs are significantly enhanced in water. A series of colloidal complex fluids by mixing PEG grafted ZIF-8 (i. e. PEG-g-ZIF-8) NPs with different amounts of polyvinylalcohol (PVA) was prepared and characterized by advanced characterization tools such as dynamic light scattering (DLS) and small-angle X-ray scattering (SAXS) thereby showing their long-term colloidal stability. Finally, dense and supported mixed matrix membranes were cast from PEG-g-ZIF-8/PVA solutions and have shown high performance in isopropanol (IPA) dehydration by pervaporation. The permeation flux of the supported MMM (i. e. 0.091 kg/(m 2 h) is eleven times higher than that of the pure PVA membrane and these MMMs present a high separation factor (i. e. 7326). These transport properties are presumably due to the molecular sieving effects induced by ZIF-8 and the good interfacial properties of the membrane. The computational exploration of the ZIF-8/PVA and PEG/PVA interfaces provides a microscopic scale explanation for the enhanced compatibility of PVA with the PEGylated MOF when compared to that for the composite based on the bare ZIF-8 as a filler.
In 1996 Sir Harold W. Kroto, Robert F. Curl and Richard E. Smalley were honored with the Nobel Prize in Chemistry for the discovery of fullerenes. The advent of these new forms of carbon heralded a race to understand the physical and chemical properties. C 60 is virtually insoluble in polar solvents but is partially soluble in benzene, toluene, and carbon disulfide. This made the processing of fullerenes for new applications fairly problematic. However, the physical and chemical properties of these cage structures may be tailored for a wide range of applications. Some of the difficulties in processing have been overcome by using novel fullerene derivatives. The functionalization of the fullerene core with different chemical moieties provided a vector toward potential applications in drug delivery, optoelectronics, electrochemistry and organic photovoltaics. In this review, we will take a closer look at the features of some of the fullerene derivatives that have reinvigorated the field of fullerene research. Water-soluble polyhydroxylated fullerenes such as fullerenol have demonstrated the potential for good electron transfer and optical transmission, while hydrophobic fullerene derivatives have shown promising avenues for catalytic applications. 2015 marked the 30 th anniversary of the discovery of fullerenes, with celebrations around the world including an event by the Royal Society of Chemistry, bringing together many of Sir Harold Kroto's former students. The event also coincided with the recent discovery of C 60 + in space after a complex twenty-year search. It is with sadness that we, Harry's Research Group at Florida State University, and his international collaborators, reflect on the passing of Sir Harold Kroto. His dedication to science and commitment to science communication through the VEGA Science Trust and the Global Educational Outreach for Science Engineering and Technology (GEOSET) initiative help to raise awareness of the challenges for science in the modern world. We will continue to inspire young students through outreach activities he initiated. Nanostructured carbon materials including fullerenes, carbon nanotubes, graphene and carbon black have the potential to be transformative in many areas from medicine to engineering. Research into carbon nanotubes is diverse in areas such as electrochemical devices, field emission, sensors and probes. [1][2][3][4] Recently, carbon nanotubes have been used as additives in the thermoplastics typically used for 3D printing. 5,6 Graphene is the latest material to have peaked interest in the carbon field in a similar manner to carbon nanotubes, with a range of potential applications.7 Graphene oxide is being explored in the production of 3D holographic images. 8The famous paper in Nature, C60:Buckminsterfullerene, 9 introduced the world to the new form of carbon but the road to general acceptance at that time was difficult, even with mounting evidence in support of the discovery. The paper, now cited over 10,000 times has become the central point of referen...
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