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At least 1,531 records · Page 85Linked to original sources
PubMed2006

Field-effect sensors with charged macromolecules: characterisation by capacitance-voltage, constant-capacitance, impedance spectroscopy and atomic-force microscopy methods.

Field-effect-based capacitive electrolyte-insulator-semiconductor (EIS) sensors have been utilised for the deoxyribonucleic acid (DNA) immobilisation and hybridisation detection as well as for monitoring the layer-by-layer adsorption of polyelectrolytes (anionic poly(sodium 4-styrene sulfonate) (PSS) and cationic poly(allylamine hydrochloride) (PAH)). The EIS sensors with charged macromolecules have been systematically characterised by capacitance-voltage, constant-capacitance, impedance spectroscopy and atomic-force microscopy methods. The effect of the number and polarity of the polyelectrolyte layers on the shift of the capacitance-voltage curves has been investigated. Alternating potential shifts of about 30-90 mV have been observed after the adsorption of each polyanion and polycation layer, respectively. The DNA immobilisation and hybridisation signals were 35-55 and 24-33 mV, respectively. The possible mechanisms for the sensor responses are discussed.

DNA↗
PubMed2005

Examination of soil contaminated by coal-liquids by size exclusion chromatography in 1-methyl-2-pyrrolidinone solution to evaluate interference from humic and fulvic acids and extracts from peat.

Soil from a redundant coke oven site has been examined by extraction of soluble materials using 1-methyl-2-pyrrolidinone (NMP) followed by size exclusion chromatography (SEC) of the extracted material. The extracted material was found to closely resemble a high temperature coal tar pitch. Standard humic and fulvic acids were also examined since these materials are very soluble in NMP and would be extracted with pitch if present in the soil. Humic substances derived from peat samples and NMP-extracts of peats were also examined. The results show that the humic and fulvic substances were not extracted directly by NMP from peats. They were extracted using caustic soda solution and were different from the peat extracts in NMP. These results indicate that humic and fulvic acids were soluble in NMP in the protonated polyelectrolyte form but not in the original native polyelectrolyte form. The extraction of soil using NMP followed by SEC appears to be a promising method for identifying contamination by coal-based industries.

Benzopyrans↗
PubMed2005

On the role of methacrylic acid copolymers in the intracellular delivery of antisense oligonucleotides.

The delivery of active biomacromolecules to the cytoplasm is a major challenge as it is generally hindered by the endosomal/lysosomal barrier. Synthetic titratable polyanions can overcome this barrier by destabilizing membrane bilayers at pH values typically found in endosomes. This study investigates how anionic polyelectrolytes can enhance the cytoplasmic delivery of an antisense oligonucleotide (ODN). Novel methacrylic acid (MAA) copolymers were examined for their pH-sensitive properties and ability to destabilize cell membranes in a pH-dependent manner. Ternary complex formulations prepared with the ODN, a cationic lipid and a MAA copolymer were systematically characterized with respect to their size, zeta potential, antisense activity, cytotoxicity and cellular uptake using the A549 human lung carcinoma cell line. The MAA copolymer substantially increased the activity of the antisense ODN in inhibiting the expression of protein kinase C-alpha. Uptake, cytotoxicity and antisense activity were strongly dependent on copolymer concentration. Metabolic inhibitors demonstrated that endocytosis was the major internalization pathway of the complexes, and that endosomal acidification was essential for ODN activity. Confocal microscopy analysis of cells incubated with fluorescently-labeled complexes revealed selective delivery of the ODN, but not of the copolymer, to the cytoplasm/nucleus. This study provides new insight into the mechanisms of intracellular delivery of macromolecular drugs, using synthetic anionic polyelectrolytes.

Active Transport, Cell Nucleus↗
PubMed2004

Determination of fiber charge components of Lo-solids unbleached kraft pulps.

Four different titration methods for measurement of fiber charge were used in this study. Each method gave different fiber charge values depending on the acidity of the end point and the interaction between the fiber chemical components and the titrant. Also, the interactions between the ionizable groups on the fiber had significant effects on the interpretation of these results. The conductometric titrations showed trends similar to the results obtained from the potentiometric titration. The conductometric titrations with NaOH produced higher fiber charge values, higher than the titrations with NaHCO(3). The differences between the results obtained from the potentiometric and polyelectrolyte titrations, which were associated with the dissolved fiber components during the delignification, were linearly related to the Kappa number of pulps. The positive intercept of this linear relationship indicated that the kraft pulping process not only removed the ionizable groups associated with the dissolved components, but at the same time provided conditions to form new ionizable groups in the fibers. The polyelectrolyte titration results indicated that the lignin content in the fibers did not affect the fiber surface charge. Data extracted from the FTIR spectra of protonated fibers were highly correlated with the fiber charge values obtained from the conductometric titration with NaOH.

Journal Article↗
PubMed2004

Single particle light-scattering photometry--some fields of application.

Present developments in the field of bioscience will profit from the fabrication of multilayer films of polyelectrolytes on colloids as well as of nano- and microsized capsules. The single particle light-scattering technique is suitable for process control. This paper describes the mode of operation and efficiency of a laboratory-built single particle light-scattering photometer, which opens up new possibilities in applications, especially in the field of bioscience. This has been achieved by improving the measurement capabilities of organic particle sizes near 100 nm and precision of thickness changes of about 0.5 nm. Besides the classic applications, such as particle size distribution measurements at high resolution and the coagulation kinetics of colloids, the measurement of the layer-by-layer polyelectrolyte adsorption at colloid particle surfaces and the fabrication of colloidal carriers is introduced. The described method is also a precise method for controlling the removal of the latex core to obtain multilayer microcapsules.

Journal Article↗
PubMed2005

Recovery of nanoparticles produced in phosphatidylcholine-based template phases.

This paper focuses on the characterization and use of polymer-modified phosphatidylcholine (PC)/sodium dodecyl sulfate (SDS)-based inverse microemulsions as a template phase for BaSO4 nanoparticle formation. The area of the optically clear inverse microemulsion phase in the isooctane/hexanol/water/PC/SDS system is not significantly changed by adding polyelectrolytes, i.e., poly(diallyldimethylammonium chloride) (PDADMAC), or amphoteric copolymers of diallyldimethylammonium chloride and maleamid acid to the SDS-modified inverse microemulsion. Shear experiments show non-Newtonian flow behavior and oscillation experiments show a frequency-dependent viscosity increase (dilatant behavior) of the microemulsions. Small amounts of bulk water were identified by means of differential scanning calorimetry. One can conclude that the macromolecules are incorporated into the individual droplets, and polymer-filled microemulsions are formed. The polymer-filled microemulsions were used as a template phase for the synthesis of BaSO4 nanoparticles. After solvent evaporation the nanoparticles were redispersed in water and isooctane, respectively. The polymers incorporated into the microemulsion are involved in the redispersion process and influence the size and shape of the redispersed BaSO4 particles in a specific way. The crystallization process mainly depends on the type of solvent and the polymer component added. In the presence of the cationic polyelectrolyte PDADMAC the crystallization to larger cubic crystals is inhibited, and layers consisting of polymer-stabilized spherical nanoparticles of BaSO4 (6 nm in size) will be observed.

Journal Article↗
PubMed2005

Preparation and characterization of polymer composite multilayers on SiO2.

Poly(diallyldimethylammonium chloride) (PDADMAC) and poly(sodium 4-styrenesulfonate) (PSS) have been consecutively adsorbed onto 1.5-microm charged silica (SiO2) particles. Time-dependent adsorption studies indicate that, due to the strong ionic charge of the dissociated polycation in water, adsorption is complete in less than 30 min. Indications of the maximum adsorption density, changes in surface charge, and stability of the layered particles are demonstrated through adsorption isotherms and electrophoretic mobility (EPM) measurements. Further stability of the PDADMAC layer is demonstrated through multiwashing with ultra pure deionized water. Preliminary desorption studies of the PSS layer also illustrate a stabilized two-layer system. Due to the nature of the electrostatic charges on the surface of the SiO2 core particles and both polyelectrolytes in aqueous media, the use of polyelectrolytes as layering elements serves as a model for the assembly of time-released drug delivery particle systems.

Journal Article↗
PubMed2005

Electrochemistry of ITO electrode modified by multilayer ultrathin films based on crown-shaped polyoxomolybdate.

The electrochemical multilayer films of crown-shaped polyoxomolybdate Na21{[Na5(H2O)14] intersection[Mo(V)(20)Mo(VI)(26)O134(OH)10(mu-CH3COO)4]}.CH3COONa.90H2O (Mo46) and polyelectrolytes by layer-by-layer assembly were investigated. The stable multilayer films were assembled by alternate adsorption of negatively charged POM and positively charged polyelectrolytes is from their aqueous dispersions. UV-vis spectroscopy and cyclic voltammetry were used to monitor the regular growth of the multilayer films. The multilayer films-modified ITO electrode was used for the detection of electrocatalytic activity toward the reduction of nitrite, bromate, and hydrogen peroxide. The proposed novel immobilized method exhibited good stability, reproducibility and high sensitivity for the determination of electrocatalytic, which is important for practical application.

Letter↗
PubMed2005

Adsorption of poly(styrene sulfonate) of different molecular weights on alpha-alumina: effect of added sodium dodecyl sulfate.

The adsorption of poly(styrene sulfonate), PSS, of different molecular weights (70,000, 500,000, and 1,000,000 mol/kg), from aqueous solutions on alpha-alumina has been investigated. PSS of the lower molecular weight adsorbs less than the others whose adsorption isotherms overlap. The adsorption is found to increase with increasing ionic strength of the solutions indicating that both electrostatic and non-electrostatic contributions are involved in the adsorption process. Upon addition of the anionic surfactant, sodium dodecyl sulfate, SDS, PSS is found to adsorb less the more SDS added. SDS is found to be preferentially adsorbed as shown both from the simultaneous adsorption of the components and also from the sequential adsorption process where SDS in all cases displaces preadsorbed PSS from the solid surface. The displacement of preadsorbed polyelectrolyte by surfactant is a very slow process and the displacement is less pronounced as the molecular mass of the polyelectrolyte increases indicating the fewer number of contact points to the surface. This is further underlined by the effect on the displacement of PSS by SDS upon increasing the ionic strength of the solutions.

Journal Article↗
PubMed2005

Effect of molecular weight and degree of deacetylation of chitosan on the formation of oil-in-water emulsions stabilized by surfactant-chitosan membranes.

The objective of this study was to establish the influence of polyelectrolyte characteristics (molecular weight and charge density) on the properties of oil-in-water emulsions containing oil droplets surrounded by surfactant-polyelectrolyte layers. A surfactant-stabilized emulsion containing small droplets (d32 approximately 0.3 microm) was prepared by homogenizing 20 wt% corn oil with 80 wt% emulsifier solution (20 mM SDS or 2.5 wt% Tween 20, 100 mM acetate buffer, pH 3) using a high-pressure valve homogenizer. This primary emulsion was then diluted with various chitosan solutions to produce secondary emulsions with a range of chitosan concentrations (3 wt% corn oil, 0-1 wt% chitosan). The influence of the molecular characteristics of chitosan on the properties of these emulsions was examined by using chitosan ingredients with different molecular weights (MW approximately 15, 145, and 200 kDa) and degree of deacetylation (DDA approximately 40, 77, and 92%). The electrical charge and particle size of the secondary emulsions were then measured. Extensive droplet aggregation occurred when the chitosan concentration was below the amount required to saturate the droplet surfaces, but stable emulsions could be formed at higher chitosan concentrations. The zeta-potential and mean diameter (d32) of the particles in the secondary emulsions was not strongly influenced by chitosan MW, however the chitosan with the lowest DDA (40%) produced droplets with smaller mean diameters and zeta-potentials than the other two DDA samples examined. Interestingly, we found that stable multilayer emulsions could be formed by mixing medium or high MW chitosan with an emulsion stabilized by a non-ionic surfactant (Tween 20) due to the fact the initial droplets had some negative charge. The information obtained from this study is useful for preparing emulsions stabilized by multilayer interfacial layers.

Chitosan↗
PubMed2006

Stable oxide nanoparticle clusters obtained by complexation.

We report on the electrostatic complexation between polyelectrolyte-neutral copolymers and oppositely charged 6-nm crystalline nanoparticles. For two different dispersions of oxide nanoparticles, the electrostatic complexation gives rise to the formation of stable nanoparticle clusters in the range 20-100 nm. It is found that inside the clusters, the particles are "pasted" together by the polyelectrolyte blocks adsorbed on their surface. Cryo-transmission electronic microscopy allows visualization of the clusters and determination of the probability distribution functions in size and in aggregation number. The comparison between light scattering and cryo-microscopy results suggests the existence of a polymer brush around the clusters.

Journal Article↗
PubMed2006

Characterization limits of a polymer adsorbed under a monolayer by GIXD measurements.

The study of interactions between a polyelectrolyte (sodium polystyrene sulfonate, PSSt) or its water-soluble monomer (SSt) at different concentrations and a monolayer of dioctadecyldimethylammonium bromide (DODA) has been investigated. The monolayer phase behavior and structure at the air-water interface were studied by surface pressure-area isotherms and grazing incidence X-ray diffraction measurements. DODA molecules organize following a rectangular unit cell in all three subphases (pure water, water containing SSt or PSSt). The presence of polyelectrolytes in the subphase decreases, on one hand, the tilt angle and the mean area per molecule in the condensed phase, revealing a higher 2D density in this state, and, on the other hand, the amount of organized matter.

Journal Article↗
PubMed2004

Correlation of transdermal iontophoretic phenylalanine and mannitol transport: test of the internal standard concept under DC iontophoresis and constant resistance AC iontophoresis conditions.

The purpose of this study was to test the feasibility of using an internal standard approach to predict the transdermal flux of phenylalanine (Phe) across human epidermal membrane (HEM) in vitro during iontophoresis of constant direct current (DC), constant skin resistance alternating current (AC) with DC offset (AC-plus-DC), symmetric constant resistance AC (AC-only), and constant current DC with the application of a polyelectrolyte. Under the constant current DC and AC-plus-DC conditions, a linear relationship between the permeation of Phe and that of mannitol was observed with a slope close to unity. The ratios of the Phe permeability coefficients to those of mannitol during iontophoresis with different HEM samples were essentially constant with significantly smaller inter-sample and intra-sample variabilities than those of the raw Phe permeability coefficient data. This demonstrates that mannitol is a good internal standard for predicting the transdermal iontophoretic flux of Phe under these two conditions. On the other hand, the correlations of the permeability coefficients of Phe and mannitol under the AC-only iontophoresis and iontophoresis with the polyelectrolyte are poorer than those observed during DC and AC-plus-DC iontophoresis. The poor correlations are believed to be related to Phe being a zwitterion and its anionic form in HEM. Previously, iontophoretic transport of glucose has been demonstrated to be essentially the same as that of mannitol. The good correlations between Phe and mannitol transport across HEM during DC and AC-plus-DC iontophoresis in the present study therefore suggest that glucose and its extraction can be used as the internal standard for iontophoretic Phe monitoring.

Administration, Cutaneous↗
PubMed2006

Scaling filtration time initial dependencies of wastewater sludges.

The filtration time, t(f), during constant pressure dead-end filtration testing of wastewater sludge is dependant on the initial height, h(0), and the initial solids concentration, phi(0). The theoretical dependencies of these initial conditions are explored: t(f) varies with h(0)(2) and cphi(0)(2), where c is a material dependant parameter that is also dependant on phi(0) and the applied pressure. Empirical values for c relative to a given phi(0) are determined from phenomenological filtration theory to give a qualitative scaling method to compare the filtration behaviour of highly compressible materials under differing initial conditions. The method is validated using filtration testing of municipal wastewater sludge. This new scaling method is applied to the filtration results of a range of different wastewater sludges, additives and treatments to illustrate its application for plant comparisons, polyelectrolyte comparisons, dose optimisation of polyelectrolyte and ferric chloride and combinations thereof, and the effects of two physicochemical treatments.

Filtration↗
PubMed2001

Diffusing probe measurements in Newtonian and elastic solutions.

The diffusion coefficients of polystyrene latex spheres and hematite particles in both Newtonian and elastic liquids have been measured using dynamic light scattering. The diffusion coefficients of the latex particles measured in glycerol/water (Newtonian) solutions obey Stokes-Einstein behaviour over a range of solvent viscosities and temperatures. Two apparent diffusion coefficients for the particles are measured in visco-elastic polyacrylamide and polyacrylate solutions and are designated Dfast and Dslow. The apparent fast diffusion coefficients measured in the elastic solutions show an increase to a maximum, above that measured in the solvent water, with increasing polyelectrolyte concentration. At higher polyelectrolyte concentrations the observed Dfast values decrease below the value obtained in the solvent water. Dfast increases with the scattering vector squared (q2) while Dslow, is independent of q2.

Journal Article↗
PubMed2003

Langmuir monolayers to study interactions at model membrane surfaces.

Langmuir monolayers at the liquid-air interface are well-defined interfacial systems and, therefore, excellent model systems to learn about interactions at interfaces beyond the classical DLVO description. Many parameters can be independently varied over a broad range and the structure can be analyzed with A precision. In the first part of the paper, the rich polymorphism in monolayers composed of amphiphilic molecules is demonstrated. Using homologues series generic phase diagrams can be derived. The delicate interplay of interactions causes a richness of phases which in turn can be used to measure fine variations in these interactions. Based on the understanding of the polymorphism in pure or mixed lipid monolayers, one can study the interaction of molecules dissolved in the subphase with monolayers. Samples presented are chemical reactions catalyzed by enzymes and coupling of polyelectrolytes to oppositely charged monolayers. To relate structure and reactivity, the activity of enzymes at the interface can be studied, predominantly combining X-ray diffraction and FTIR-spectroscopy. It is shown that the activity depends on monolayer structure. In one case, the reaction product leads to structural changes in the monolayer and stops the reaction, hence, indicating a subtle case of product inhibition via the membrane. On the other hand it has become possible to manipulate the organization of polyelectrolytes at interfaces via lipid charge density and ionic strength. In the most important case of DNA interacting with a membrane surface we show that DNA arranges at the interface in a lamellar manner, and the intermolecular distances, measured by Synchrotron X-ray diffraction can be varied by the lipid density.

Adsorption↗
PubMed1998

Red blood cell shape as a function of medium's ionic strength and pH.

Glycocalyx, the characteristic first line of interaction between membrane and environment, can be visualized as a polyelectrolyte anchored to a bending-resistant matrix. This structure has an amazing resemblance with the ionized monolayers, in which, the cohesion among hydrocarbon chains is counteracted by the repulsion among similarly charged ionic heads, and thus the balance determines the curvature of the membrane. Likewise, it could be assumed that in biological membranes, repulsion among similarly charged groups in the glycocalyx could generate different curving trends. Hence, the factors directly influencing the electrostatic interaction among surface charged groups were studied, assessing the effect of the medium's ionic strength (mu) and pH, in an extensive range of values around the physiological one. The results point out mu variations inducing different shapes, depending on whether mu values were lower or higher than the physiological ones; which could be explained by the polyelectrolyte theory. The occurrence of more invaginated shapes as the medium's pH decreases, and the opposite event, when the pH increases, could be attributed to the coupling between the dissociation of the glycocalyx ionic groups and the H+ concentration. The behavior of the cells with reduced surface charges (by neuraminidase degradation) supports the hypothesis that the observed mu and the pH effect on erythrocyte shape could be mediated by glycocalyx charged groups.

Adult↗
PubMed2000

A commentary on the screened-Oseen, counterion-condensation formalism of polyion electrophoresis.

The use of linear theory, in particular, counterion condensation (CC) theory, in describing electrophoresis of polyelectrolyte chains, is criticized on several grounds. First, there are problems with CC theory in describing the equilibrium distribution of ions around polyelectrolytes. Second, CC theory is used to treat ion relaxation in a linear theory with respect to the polyion charge despite the fact that ion relaxation arises as a consequence of nonlinear charge effects. This nonlinearity has been well established by several investigators over the last 70 years for spherical, cylindrical, and arbitrarily shaped model polyions. Third, current use of CC theory ignores the electrophoretic hindrance as well as the ion relaxation for condensed counterions and only includes such interactions for uncondensed counterions. Because most of the condensed counterions lie outside the shear surface of the polyion (in the example of DNA), the assumption of ion condensation is artificial and unphysical. Fourth, the singular solution, based on a screened Oseen tensor, currently used in the above mentioned theories is simply wrong and fails to account for the incompressibility of the solvent. The actual singular solution, which has long been available, is discussed. In conclusion, it is pointed out that numerical alternatives based on classic electrophoresis theory (J.T.G. Overbeek, Kolloid-Beih, 1943, 54:287-364) are now available.

Biopolymers↗