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This work describes the encapsulation of hydrogen storage materials from organic solvents. Due to complex formation the shell provides stability and selective permeability. Specifically, sodium borohydride particles were encapsulated within polymer films by the layer-by-layer self-assembly of oppositely charged polyelectrolytes (polyethyleneimine and poly(acrylonitrile-co-butadiene-co-acrylic acid)). The polymer nanofilm fabrication was performed using dichloromethane as a working media. IR spectroscopy was applied to investigate the chemical interaction between the polyelectrolytes. The multilayer film preparation was verified by Z-potential measurements, scanning electron microscopy, and confocal laser microscopy. The stability of sodium borohydride protected with a polyelectrolyte shell was increased compared to that of the pure material under ambient conditions.
ACS Appl Mater Interfaces 2009 May
PMID:Polyelectrolyte multilayered nanofilms as a novel approach for the protection of hydrogen storage materials. 2035 84

Polydiacetylene (PDA)-doped calcium alginate fibers were created by the solution blending of polymerized 10,12-pentacosadiynoic acid liposomes with sodium alginate in water prior to extrusion. The liposomes maintained their blue color during wet spinning and drying of the fibers but changed to red with exposure to specific external stimuli (heat, solvent, and chemical). In the latter case, the color change only occurred when the fibers were sufficiently permeable for the reacting species to reach the interior. A parameter termed the "Raman response" (RR) has been developed to quantify the amount of PDA liposomes in each of two critical conformations within the fibers. The RR attributes a quantitative measure of PDA response to individual stimuli. This method provides advantages over the commonly used "colorimetric response" in systems where sample limitations and chromophore activity make UV-vis spectroscopic measurements difficult or inaccurate. PDA liposomes are shown to effectively add a versatile sensing component to alginate fibers.
ACS Appl Mater Interfaces 2009 Jun
PMID:Preparation, characterization, and sensing behavior of polydiacetylene liposomes embedded in alginate fibers. 2035 25

The hydration of the surface of a highly bioactive silicate glass was modeled using ab initio (Car-Parrinello) molecular dynamics (CPMD) simulations, focusing on the structural and chemical modifications taking place at the glass-water interface immediately after contact and on the way in which they can affect the bioactivity of these materials. The adsorption of a water dimer and trimer on the dry surface was studied first, followed by the extended interface between the glass and liquid water. The CPMD trajectories provide atomistic insight into the initial stages relevant to the biological activity of these materials: following contact of the glass with an aqueous (physiological) medium, the initial enrichment of the surface region in Na+ cations establishes dominant Na+-water interactions at the surface, which allow water molecules to penetrate into the open glass network and start its partial dissolution. The model of a Na/H-exchanged interface shows that Ca2+-water interactions are mainly established after the dominant fraction of Na is leached into the solution. Another critical role of modifier cations was highlighted: they provide the Lewis acidity necessary to neutralize OH(-) produced by water dissociation and protonation of nonbridging oxygen (NBO) surface sites. The CPMD simulations also highlighted an alternative, proton-hopping mechanism by which the same process can take place in the liquid water film. The main features of the bioactive glass surface immediately after contact with an aqueous medium, as emerged from the simulations, are (a) silanol groups formed by either water dissociation at undercoordinated Si sites or direct protonation of NBOs, (b) OH(-) groups generally stabilized by modifier cations and coupled with the protonated NBOs, and (c) small rings, relatively stable and unopened even after exposure to liquid water. The possible role and effect of these sites in the bioactive process are discussed.
ACS Appl Mater Interfaces 2009 Jun
PMID:Modeling the water-bioglass interface by ab initio molecular dynamics simulations. 2035 29

Freestanding quasi-two-dimensional ultrathin films (e.g., 41 nm thick polymer nanosheets) were produced, on which stimuli-responsive 47 nm thick polymer brushes were constructed by atom transfer radical polymerization (ATRP) of poly(N-isopropylacrylamide). The resulting surfaces of the multilayered polysaccharide ultrathin films were evaluated by ellipsometry, IR imaging, in situ variable-temperature atomic force microscopy (AFM), and contact angle measurements. The morphological transformation of the freestanding polymer nanosheet bearing thermoresponsive polymer brushes was observed macroscopically through reversible structural color changes at the air-water interface. The dynamic shape change of the nanosheet was also monitored with the addition of a surfactant such as sodium n-dodecylsulfate to reduce the hydrophobicity of the surface. It was then demonstrated that the highly flexible freestanding polymer nanosheet is capable of acting as a unique platform for inducing stimuli-responsive behavior in nanomaterials.
ACS Appl Mater Interfaces 2009 Jul
PMID:Hydrodynamic transformation of a freestanding polymer nanosheet induced by a thermoresponsive surface. 2035 42

Alkali etching of a poly(l-lactic acid) fiber was studied by exposing the fiber surface to sodium hydroxide solutions. The factors examined included the etching time (0-1.5 h), alkali concentration (0.25-3 mol/L), and etching temperature (25-80 degrees C). The extent of etching was determined gravimetrically. Both weight loss and mechanical testing results suggest that alkali etching is strictly a surface hydrolysis reaction, as opposed to a bulk reaction, and thus the weight loss rate decreases with a shrinking fiber radius. A slight increase in the fiber crystallinity observed from thermal analysis was interpreted as a result of surface-limited etching on a sheath-core fiber microstructure. The dependence of the rate on the alkali concentration is nonlinear, suggesting that the fiber weight loss rate is subject to both chemical hydrolysis and transport limitations. The dependence of the rate on the temperature follows the Arrhenius equation. The fiber weight after etching can thus be predicted by an overall expression combining all factors: time, temperature, concentration, and fiber diameter.
ACS Appl Mater Interfaces 2009 Jul
PMID:Alkali etching of a poly(lactide) fiber. 2035 63

Mixtures of cationic guar (cat-guar) or cationic hydroxyethylcellulose (cat-HEC) with the anionic surfactants sodium dodecyl sulfate or sodium lauryl ether-3 sulfate have been investigated by a wide range of complementary techniques (phase studies, turbidity measurements, dynamic light scattering, gel-swelling experiments, and in situ null ellipsometry), with the following objectives in mind: (1) to establish the relationship between the bulk phase behavior (precipitation and redissolution) of the polyion/surfactant ion complexes and formation/deposition of such complexes at silica surfaces and (2) to obtain molecular interpretations of the large, previously unresolved, quantitative differences between the various investigated mixtures. There were clear similarities, for each studied system, between the bulk phase behavior, gel swelling, and surface deposition on increasing surfactant concentration. This is because all phenomena reflect the polyion/surfactant ion binding isotherm: an initial binding step at a low critical association concentration (cac) of the surfactant and a second more-or-less cooperative binding step beginning at a second cac, the cac(2). The details of the interactions are system-specific, however, and cat-guar/surfactant mixtures generally had larger precipitation regions and gave rise to larger adsorbed amounts on silica compared to mixtures with cat-HEC of a similar charge density. The observed quantitative differences are attributed to a difference in the hydrophobicity of the polyions. For cat-guar, the comparatively weak hydrophobic polyion/surfactant attraction is seen as a very gradual binding commencing at the cac(2) and continuing past the bulk critical micelle concentration of the surfactant, resulting in an unusually large phase-separation region. For cat-HEC, the dissolution of the precipitate takes place at lower surfactant concentrations because of a stronger hydrophobic interaction between the surfactant and the polyion. The results have implications for the successful design of oppositely charged polyelectrolyte/surfactant formulations for surface deposition applications.
ACS Appl Mater Interfaces 2009 Nov
PMID:Surface deposition and phase behavior of oppositely charged polyion/surfactant ion complexes. 1. Cationic guar versus cationic hydroxyethylcellulose in mixtures with anionic surfactants. 2035 12

Fabrication of multilayer ultrathin composite films composed of nanosized titanium dioxide particles (P25, Degussa) and polyelectrolytes (PELs), such as poly(allyl amine hydrochloride) (PAH) and poly(styrene sulfonate sodium salt) (PSS), on glass substrates using the layer-by-layer (LbL) assembly technique and its potential application for the photodegradation of rhodamine B under ultraviolet (UV) irradiation has been reported. The polyelectrolytes and TiO(2) were deposited on glass substrates at pH 2.5 and the growth of the multilayers was studied using UV/vis spectrophotometer. Thickness measurements of the films showed a linear increase in film thickness with increase in number of bilayers. The surface microstructure of the thin films was characterized by field emission scanning electron microscope. The ability of the catalysts immobilized by this technique was compared with TiO(2) films prepared by drop casting and spin coating methods. Comparison has been made in terms of film stability and photodegradation of rhodamine B. Process variables such as the effect of surface area of the multilayers, number of bilayers, and initial dye concentration on photodegradation of rhodamine B were studied. Degradation efficiency increased with increase in number of catalysts (total surface area) and bilayers. Kinetics analysis indicated that the photodegradation rates follow first order kinetics. Under maximum loading of TiO(2), with five catalyst slides having 20 bilayers of polyelectrolyte/TiO(2) on each, 100 mL of 10 mg/L dye solution could be degraded completely in 4 h. The same slides could be reused with the same efficiency for several cycles. This study demonstrates that nanoparticles can be used in wastewater treatment using a simple immobilization technique. This makes the process an attractive option for scale up.
ACS Appl Mater Interfaces 2009 Nov
PMID:LbL fabricated poly(styrene sulfonate)/TiO(2) multilayer thin films for environmental applications. 2035 43

Chiral polyelectrolyte multilayers (PEMs) consisting of poly(l-lysine) (PLL), poly(N-(S)alkylated 4-vinylpyridinium iodide), or poly(ethyleneimine maltose) (PEI-m) as polycations and poly(styrenesulfonic acid) sodium salt (PSS) or poly(vinyl sulfate) as polyanions, as well as a nonchiral PEM composed of poly(ethyleneimine) (PEI) and PSS were deposited on silicon substrates and poly(tetrafluoroethylene) membranes using the layer-by-layer method. For these PEMs, enantiospecific interaction toward one enantiomer of either l/d-glutamic acid (l/d-GLU), l/d-tryptophan, or l/d-ascorbic acid (l/d-ASC), respectively, was studied under variation of the concentration, pH, and ionic strength. Both deposition and enantiospecific interaction were analyzed by attenuated total reflection Fourier transform infrared spectroscopy. Our results show a significant enantiospecific preference of d-GLU over l-GLU at PEMs containing PLL and of d-ASC over l-ASC at PEMs containing PEI-m. No such enantiospecific preference was found for nonchiral PEMs containing PEI. The enantiospecificity of PEMs of PLL/PSS toward l/d-GLU could be significantly influenced by the ionic strength and pH values, so that increasing attractive electrostatic interactions resulted in higher enantiospecificity.
ACS Appl Mater Interfaces 2009 Dec
PMID:In situ ATR-FTIR investigation on the preparation and enantiospecificity of chiral polyelectrolyte multilayers. 2035 70

Electrostatic layer-by-layer assembly was the basis for the synthesis of multilayer nanorod/polymer composite films. Cationic and water-soluble CdSe nanorods (NRs) were synthesized and partnered with anionic polymers including poly(sodium 4-styrenesulfonate) (PSS) and two polythiophene-based photoactive polymers, sodium poly[2-(3-thienyl)-ethoxy-4-butylsulfonate (PTEBS) and poly[3-(potassium-6-hexanoate)thiophene-2,5-diyl] (P3KHT). Controlled multilayer growth is shown through UV-vis spectroscopy, cross-sectional SEM and surface analytical techniques including atomic force microscopy. The formation of an intimate nanorod/conducting polymer bulk heterojunction is confirmed through cross-sectional SEM, TEM, and scanning Auger analysis. A series of photovoltaic devices was fabricated on ITO electrodes using CdSe NRs in combination with PTEBS or P3KHT. A thorough device analysis showed that performance was limited by low short circuit current although charge transfer was confirmed in the ELBL nanocomposite thin films.
ACS Appl Mater Interfaces 2010 Jan
PMID:Electrostatic layer-by-layer assembly of CdSe nanorod/polymer nanocomposite thin films. 2035 38

An alternative approach for the creation of proton conducting platforms is presented. The methodology is based on the so-called "pore-filling concept", which relies on the filling of porous matrices with polyelectrolytes to obtain proton conducting platforms with high dimensional stability. Polymer-silicon composite membranes, with well-defined polyelectrolyte microdomains oriented normal to the plane of the membrane, were prepared using photoelectrochemically etched silicon as a microstructured scaffold. Ordered two-dimensional macroporous silicon structures were rendered proton conducting by filling the micropores via a surface-initiated atom transfer radical polymerization process. The morphological aspects, chemical stability, and performance of the hybrid assemblies were characterized by a set of techniques including scanning electron microscopy, Fourier transform infrared spectroscopy, X-ray photoelectron spectroscopy, nuclear magnetic resonance and impedance spectroscopy, among others. The fabricated silicon-poly(sodium 2-acrylamide-2-methylpropane sulfonate) hybrid membranes displayed proton conductivities in the range of 1x10(-2) S/cm. This work illustrates the potential of hybrid polymer-silicon composite membranes synthesized by pore-filling surface-initiated polymerization to create proton conducting platforms in a simple and straightforward manner. Versatility and relative ease of preparation are two key aspects that make this approach an attractive alternative for the molecular design and preparation of proton conducting systems.
ACS Appl Mater Interfaces 2010 Jan
PMID:Hybrid polymer-silicon proton conducting membranes via a pore-filling surface-initiated polymerization approach. 2035 46


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