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PubMed2002

Investigation of pseudoisocyanine aggregates formed on polystyrenesulfonate.

The interaction of 1,1'-diethyl-2,2'-cyanine (PIC), a non-fluorescent cationic dye known to form emissive J-aggregates in aqueous solutions, with the polyelectrolyte poly(styrenesulfonate) (PSS) is investigated by absorption and fluorescence spectroscopy. Depending on the amount of polyelectrolyte added, three regimes are identified. At a large excess of PIC, there is an equilibrium between the PIC monomer and a non-fluorescent PIC aggregate characterized by a strong absorption band centered at 565 nm. As the amount of PSS increases, we observe the growth of the PIC J-aggregate onto the PSS backbone, characterized by a sharp absorption band at 572 nm and a narrow emission at 577 nm. At a large excess of PSS, the major species consists of PIC molecules adsorbed independently along the polyelectrolyte chains.

Journal Article↗
PubMed2005

Self-organization of cationic dendrimers in polyanionic hydrogels.

Protonated poly(propylene imine) dendrimers (Astramol) of five generations: DAB-dendr-(NH2)x (where x=4, 8, 16, 32 or 64) are sorbed by slightly cross-linked polyanionic hydrogels: poly(sodium acrylate) and poly(sodium 2-acrylamido-2-methylpropane sulfonate). As a result highly swollen original hydrogel transforms into compact cross-linked polyelectrolyte-dendrimer complexes. Sorption of dendrimers by the hydrogels is a chemically drawn frontal diffusion process. Driving force comes from the gain in the free energy of interpolyelectrolyte coupling reaction between the charged dendrimer molecules and the oppositely charged hydrogel network, accompanied with entropically favourable release of low molecular salt into environment. The amount of a simple salt released is equivalent to a number of intermolecular salt bonds, formed between protonated dendrimers and hydrogel networks. Apparently the mechanism of dendrimer uptake involves a "relay-race" transfer of dendrimer polycations from one fragment of polyelectrolyte network to the other via interpolyelectrolyte exchange reaction. As a result "core-shell" constructs consisting of outer weakly swollen complex shell and highly swollen hydrogel core are formed at intermediate stages of the process. The rate of sorption is determined by the rate of the interpolyelectrolyte exchange reaction that is the rate of the formation of free fragments of polyelectrolyte network (vacancies) on the inner complex-hydrogel boundary. The amount of vacancies depends on the area of this boundary. Consequently kinetics of dendrimer uptake could not be fitted in terms of Fickian diffusion (except DAB-dendr-(NH2)4), but expressed in terms of the kinetic equation derived for a frontal heterogeneous reaction. Sorbed dendrimers of all studied generations at pH values ensuring complete protonation of primary and tertiary amine groups are closely packed in hydrogel networks, so that all dendrimer cationic units form ion pairs with anionic units of hydrogels. In other words polyanionic network fragments are able to penetrate into the interior of fully protonated DAB-dendr-(NH2)x species as it was earlier shown for flexible linear polyanions. In such case the ultimate amount of sorbed dendrimer molecules is always determined by the condition n(a)/N- = 1, where n(a) is the total number of dendrimer amine groups, N- is the number of the anionic hydrogel units. The latter is also true for the complex shell composition in the heterogeneous reacting samples formed at intermediate stages of dendrimers uptake. Variation of pH and sorption extent is an effective tool to control dendrimer distribution, self-organization and the final structure of dendrimer-hydrogel constructs.

Journal Article↗
PubMed2005

Responsive brushes and gels as components of soft nanotechnology.

Progress in the development of generic molecular devices based on responsive polymers is discussed. Characterisation of specially synthesised polyelectrolyte gels, "grafted from" brushes and triblock copolymers is reported. A Landolt pH-oscillator, based on bromate/ sulfite/ferrocyanide, with a room temperature period of 20 min and a range of 3.1 < pH < 7.0, has been used to drive periodic oscillations in volume in a pH responsive hydrogel. The gel is coupled to the reaction and changes volume by a factor of at least 6. A continuously stirred, constant volume, tank reactor was set-up on an optical microscope and the reaction pH and gel size monitored. The cyclic force generation of this system has been measured directly in a modified JKR experiment. The responsive nature of polyelectrolyte brushes, grown by surface initiated ATRP, have been characterised by scanning force microscopy, neutron reflectometry and single molecule force measurements. Triblock copolymers, based on hydrophobic end-blocks and either polyacid or polybase mid-block, have been used to produce polymer gels where the deformation of the molecules can be followed directly by SAXS and a correlation between molecular shape change and macroscopic deformation has been established. The three systems studied allow both the macroscopic and a molecular response to be investigated independently for the crosslinked gels and the brushes. The triblock copolymers demonstrate that the individual response of the polyelectrolyte molecules scale-up to give the macroscopic response of the system in an oscillating chemical reaction.

Journal Article↗
PubMed2004

An algal removal using a combination of flocculation and flotation processes.

The paper describes certain facets of the removal of the algae (Scenedesmus quadricauda) from water, using a froth flotation separation method, in conjunction with two types of surfactants, (cetyltrimethylammonium bromide) CTAB and (sodium dodecylsulfate) SDS. A 90% algal removal efficiency was achieved when 100 mg l(-1) of CTAB was used whereas for the SDS solutions, the same concentration gave, by comparison, a very poor algal removal efficiency. An addition of 1 mg l(-1) of a commercial cationic polyelectrolyte, which was the optimal concentration as was evident from the zeta potential and the particle size distribution measurements, prior to the SDS addition resulted in a formation of algal flocs and consequently a substantial improvement in the extent of the algal removal. A 50 mg l(-1) solution of SDS was found to be the optimal concentration to completely remove these algal flocs from water. The amount of water removed along with the algal flocs, produced using 1 mg l(-1) of the commercial polyelectrolyte and subsequently removed using SDS, was comparatively lower than that removed with the algal cells when CTAB was used as the 'collector'. It was generally found, in this study, that an addition of the polyelectrolyte improved the removal efficiencies and the rate of separation and also decreased the amount of the associated water removed along with the algal sludge.

Cetrimonium↗
PubMed2005

Enhancement of organic removals in high strength herbal pharmaceutical wastewater.

Herbal Pharmaceutical wastewater was subjected to physico-chemical treatment using conventional coagulants individually and in combination with different anionic, cationic and nonionic polyelectrolytes. Results indicate cationic polyelectrolyte to be the best polymer. Individually Alum did not give good results but Alum with cationic polymer in the ratio of 300:0.25 mg l(-1) resulted in the best removals of Chemical Oxygen Demand (COD), Biochemical Oxygen Demand (BOD) and Suspended Solids (SS) of 64.0%, 69.4% and 80.82% respectively. The next combination which resulted in good removals was Lime: cationic polymer in the ratio of 300:0.20 mg l(-1) with COD, BOD, and SS removals of 57.6%, 65.1% and 74.0%, respectively. Overall the studies indicated that the herbal pharmaceutical wastewater needs to be treated by physico-chemical treatment as a primary process to reduce the organic load and increase the performance efficiency of the secondary biological treatment process. This paper discusses in detail the studies carried out using conventional coagulants along with synthetic polyelectrolyte.

Bioreactors↗
PubMed2001

Counterion evaporation.

We study the adsorption behavior of a highly charged rodlike polyelectrolyte approaching an oppositely charged planar wall in an unbounded electrolyte solution. The grand potential, the entropy, and the total number of screening particles are calculated as functions of the rod-wall distance, using input parameters that are typical of a DNA-molecule and charged lipid bilayers. It is found that counterions which are bound to the polyelectrolyte at infinite rod-wall distances will be released, or "evaporated," as the DNA molecule moves closer to the charged wall. This effect can be regarded as the opposite of the ion-condensation process. The transition of ions from the system of screening ions into the reservoir of bulk ions can lead to an increase of the enthalpy. This gain of enthalpy for the whole system manifests itself as an attractive contribution to the effective interaction between the wall and the polyelectrolyte.

Journal Article↗
PubMed2004

Spatial distribution of competing ions around DNA in solution.

The competition of monovalent and divalent cations for proximity to negatively charged DNA is of biological importance and can provide strong constraints for theoretical treatments of polyelectrolytes. Resonant x-ray scattering experiments have allowed us to monitor the number and distribution of each cation in a mixed ion cloud around DNA. These measurements provide experimental evidence to support a general theoretical prediction: the normalized distribution of each ion around polyelectrolytes remains constant when ions are mixed at different ratios. In addition, the amplitudes of the scattering signals throughout the competition provide a measurement of the surface concentration parameter that predicts the competition behavior of these cations. The data suggest that ion size needs to be taken into account in applying Poisson-Boltzmann treatments to polyelectrolytes such as DNA.

Cations↗
PubMed1982

Adsorption of reovirus by minerals and soils.

Adsorption of [35S]methionine-labeled reovirus by 30 dry soils, minerals, and finely ground rocks suspended in synthetic freshwater at pH 7 was investigated to determine the conditions necessary for optimum virus removal during land application of wastewaters. All of the minerals and soils studied were excellent adsorbents of reovirus, with greater than 99% of the virus adsorbed after 1 h at 4 degrees C. Thereafter, virus remaining in suspension was significantly inactivated, and within 24 h a three to five log10 reduction in titer occurred. The presence of divalent cations, i.e., Ca2+ and Mg2+, in synthetic freshwater enhanced removal, whereas soluble organic matter decreased the amount of virus adsorbed in secondary effluent. The amount of virus adsorbed by these substrates was inversely correlated with the amount of organic matter, capacity to adsorb cationic polyelectrolyte, and electrophoretic mobility. Adsorption increased with increasing available surface area, as suspended infectivity was reduced further by the more finely divided substrates. However, the organic content of the soils reduced the level of infectious virus adsorbed below that expected from surface area measurements alone. The inverse correlation between virus adsorption and substrate capacity for cationic polyelectrolyte indicates that the adsorption of infectious reovirus particles is predominately a charged colloidal particle-charged surface interaction. Thus, adsorption of polyelectrolyte may be useful in predicting the fate of viruses during land application of sewage effluents and sludges.

Adsorption↗
PubMed2002

Structure of colloidal complexes obtained from neutral/poly-electrolyte copolymers and oppositely charged surfactants.

We report on the phase behavior and scattering properties of colloidal complexes made from block copolymers and surfactants. The copolymer is poly(sodium acrylate)-b-poly(acrylamide), hereafter abbreviated as PANa-PAM, with molecular weight 5000 g/mol for the first block and 30000 g/mol for the second. In aqueous solutions and neutral pH, poly(sodium acrylate) is a weak polyelectrolyte, whereas poly(acrylamide) is neutral and in good-solvent conditions. The surfactant is dodecyltrimethylammonium bromide (DTAB) and is of opposite charge with respect to the polyelectrolyte block. Combining dynamical light scattering and small-angle neutron scattering, we show that in aqueous solutions PANa-PAM diblocks and DTAB associate into colloidal complexes. For surfactant-to-polymer charge ratios Z lower than a threshold (Z(C) approximately 0.3), the complexes are single surfactant micelles decorated by few copolymers. Above the threshold, the colloidal complexes reveal an original core-shell microstructure. We have found that the core of typical radius 100-200 A is constituted from densely packed surfactant micelles connected by the polyelectrolyte blocks. The outer part of the colloidal complex is a corona and is made from the neutral poly(acrylamide) chains. Typical hydrodynamic sizes for the whole aggregate are around 1000 A. The aggregation numbers expressed in terms of numbers of micelles and copolymers per complex are determined and found to be comprised between 100-400, depending on the charge ratio Z and on the total concentration. We have also shown that the sizes of the complexes depend on the exact procedure of the sample preparation. We propose that the driving mechanism for the complex formation is similar to that involved in the phase separation of homopolyelectrolyte/surfactant systems. With copolymers, the presence of the neutral blocks prevents the macroscopic phase separation from occurring.

Journal Article↗
PubMed2003

Non-linear osmotic brush regime: simulations and mean-field theory.

We investigate polyelectrolyte brushes in the osmotic regime using both theoretical analysis and molecular dynamics simulation techniques. In the simulations at moderate Bjerrum length, we observe that the brush height varies weakly with grafting density, in contrast to the accepted scaling law, which predicts a brush thickness independent of the grafting density. We show that such behavior can be explained by considering lateral electrostatic effects (within the non-linear Poisson-Boltzmann theory) combined with the coupling between lateral and longitudinal degrees of freedom due to the conserved polymer volume (which are neglected in scaling arguments). We also take the non-linear elasticity of polyelectrolyte chains into consideration, which makes significant effects as chains are almost fully stretched in the osmotic regime. It is shown that all these factors lead to a non-monotonic behavior for the brush height as a function of the grafting density. At large grafting densities, the brush height increases with increasing the grafting density due to the volume constraint. At small grafting densities, we obtain a re-stretching of the chains for decreasing grafting density, which is caused by lateral electrostatic contributions and is controlled by the counterion-condensation process around polyelectrolyte chains. These results are obtained assuming all counterions to be trapped within the brush, which is valid for sufficiently long chains of large charge fraction.

Journal Article↗
PubMed2002

Cellular target of weak magnetic fields: ionic conduction along actin filaments of microvilli.

The interaction of weak electromagnetic fields (EMF) with living cells is a most important but still unresolved biophysical problem. For this interaction, thermal and other types of noise appear to cause severe restrictions in the action of weak signals on relevant components of the cell. A recently presented general concept of regulation of ion and substrate pathways through microvilli provides a possible theoretical basis for the comprehension of physiological effects of even extremely low magnetic fields. The actin-based core of microfilaments in microvilli is proposed to represent a cellular interaction site for magnetic fields. Both the central role of F-actin in Ca2+ signaling and its polyelectrolyte nature eliciting specific ion conduction properties render the microvillar actin filament bundle an ideal interaction site for magnetic and electric fields. Ion channels at the tip of microvilli are connected with the cytoplasm by a bundle of microfilaments forming a diffusion barrier system. Because of its polyelectrolyte nature, the microfilament core of microvilli allows Ca2+ entry into the cytoplasm via nonlinear cable-like cation conduction through arrays of condensed ion clouds. The interaction of ion clouds with periodically applied EMFs and field-induced cation pumping through the cascade of potential barriers on the F-actin polyelectrolyte follows well-known physical principles of ion-magnetic field (MF) interaction and signal discrimination as described by the stochastic resonance and Brownian motor hypotheses. The proposed interaction mechanism is in accord with our present knowledge about Ca2+ signaling as the biological main target of MFs and the postulated extreme sensitivity for coherent excitation by very low field energies within specific amplitude and frequency windows. Microvillar F-actin bundles shielded by a lipid membrane appear to function like electronic integration devices for signal-to-noise enhancement; the influence of coherent signals on cation transduction is amplified, whereas that of random noise is reduced.

Actin Cytoskeleton↗
PubMed1996

The importance of standardization of carboxymethylchitin concentration by the dye-binding capacity of alcian blue before adsorption on liposomes.

A new method based on the measurement of the relative dye-binding capacity of Alcian Blue to carboxymethylchitin (CMC) at various molecular weights (MW) has been developed to facilitate the standardization of the initial polyelectrolyte concentration. In the absence of standardization, non-reproducible adsorption patterns are encountered during the adsorption of the MW CMC on neutral and positively charged liposomes. This method is sensitive down to a concentration of 5 mu g/ml of polymer in water. Static Light Scattering (SLS) measurements are used to obtain the weight average molecular weight (Mw) and the size of the polyelectrolyte (Rg) and overlap concentrations (c*). The Mws are then used to determine the constants K and a of the Mark-Houwink equation which are 1.65 x 10(-2) dl/g and 0.4701, respectively, evaluated at kappa = 0.154 M, pH = 7.4 and T = 25 degrees C. The critical electrolyte concentration decreases with molecular weight for Mws ranging from 5.0 x 10(4)-1.2 x 10(6). The dye-binding capacity changes with the molecular weight distribution of the polyelectrolyte demonstrating the sensitivity of this technique to polydispersity.

Adsorption↗
PubMed1997

Microdisperse form of immobilized hemoglobin modelling the erythrocytes.

Disperse systems based on hemoglobin sorption immobilization in reticular carboxylic polyelectrolytes are proposed as model of erythrocytes. The efficiency of oxygen transport of these systems is much higher than that of native hemoglobin and is comparable with the gas transport of erythrocytes. This is believed to be due to highly selective sorption of hemoglobin in microdisperse forms of permeable polyelectrolytes. Microparticles of immobilized hemoglobin exhibit high local concentration of hemoglobin: the protein mass being one order of magnitude than that of polymer-carrier. Besides, it is presumed that structure of the carboxylic polyelectrolyte matrix is a polymer analog of 2,3-diphosphoglycerate. Microdispersion of immobilized hemoglobin exhibits a aggregative resistance and have identity of surface charge with erythrocytes. Studies in vivo have revealed biocompatibility of immobilized hemoglobin.

Adsorption↗
PubMed2003

Investigation of selective protein immobilization on charged protein array by wavelength interrogation-based SPR sensor.

We have investigated the use of multilayer films of polyelectrolytes as selective surfaces to analyze protein interactions with a self-assembled SPR wavelength-shift sensor. Charged arrays were prepared by alternating adsorption of the charged polyelectrolytes, poly(diallyldimethylammonium chloride) (PDDA) and poly(sodium 4-styrenesulfonate) (PSS). Multilayer formation was monitored with the SPR wavelength-shift sensor and a Spreeta SPR sensor. Protein immobilization on the charged surfaces, which was also analyzed by the SPR sensors, was dependent on the pI of the proteins. Tissue transglutaminase (tTGase) and beta-galactosidase (pIs, 5.1 and 5.3, respectively) were preferentially bound to the positively charged PDDA surface, whereas lysozyme (pI, 11.0) was selectively bound to the negatively charged PSS surface. Immobilization of tTGase on the PDDA surface was also dependent on the buffer pH. The interaction of tTGase with RhoA(V14), a constitutively active form of Rho, could be detected on the charged arrays with the wavelength-shift sensor. The arrays could be reutilized at least 5 times. Thus, it is likely that charged surfaces, assembled by the layer-by-layer method using polyelectrolytes, will prove useful for preparing selective protein arrays.

Adsorption↗
PubMedDate not supplied

[Evaluation of the sanitary-and-epidemiological safety of flocculating agents used for portable water purification].

Polyelectrolytes used in the practice of water supply to the population were comparatively hygienically studied, by using a complex of hazard indices and a new approach to sanitary-and-epidemiological evaluation of the safety of water-soluble polymers is substantiated. The anionic and cationic flocculating agents from different chemical classes, such as Superflok A-100, Fennopol A 321E, Fennopol K 221E, Praestol 2530 TR, VPK-402, Superflok C-577, Saipan, KF-91, Ecosol-401, a low molecular-weight sodium polyacrylate were tested as model compounds. Moreover, the information already available in the scientific literature on the toxicity of synthetic polyelectrolytes was analyzed. The generalized maximum permissible concentrations were substantiated for individual chemical classes of synthetic polyelectrolytes: polyacrylamides, polyamines, polydiallyldimethylammonium chloride.

Acrylic Resins↗
PubMedDate not supplied

[Viral flora (coliphages and human enteroviruses) found in river water after an urban district (Saint-Etienne). I. Comparative study of four simple and inexpensive methods for concentration and isolation of river-water viruses (author's transl)].

Four methods for the concentration of human enteroviruses in the waters of the river Furan were surveyed: the original method described by WALLIS, of adsorption of viruses on PE-60 polyelectrolyte; a modified version of the Wallis method; a method using a different polyelectrolyte available in France, the POE; the two-phase system described by SHUVAL. The best results were obtained when using the method of adsorption on polyelectrolytes, and the second method was finally chosen for field surveys.

Adsorption↗
PubMed1977

[Mechanism of penicillinase inhibition by alkyl sulfates in the presence of synthetic polyeletrolytes].

Competing inhibition of Bacillus licheniformis 749/C penicillinase by alkylsulfates CnH2n+ 1OSO3N1 where n was 8--16 was studied. The values of the inhibition constants Ki of individual homologues were estimated. It was shown that stability of complex "enzyme-inhibitor" increased with lengthening of the hydrocarbon radical which was probably due to increased hydrophobic interaction of the alkyl radical with the lipophilic areas of the penicillinase active center. Inhibition in the presence of sopolymers of vinylpirrolidone with N-alkylvinylamine was studied with the aim of modeling the process of penicillinase inhibitions by alkylsulfates in the presence of the blood serum. It was shown that polyelectrolytes posessing hydrophobic substituents had an ability of reducing the activity of inhibited penicillinase, cooperative transfer of alkylsulfate molecules from the enzyme to polyelectrolyte being observed. The maximum effect was registered in the polyelectrolytes with substituents C12H25 and C16H33 which was confirmed in the experiments with the penicillinase-producing strains of staphylococci.

Alkanesulfonates↗
PubMed1985

The role of surface charge on the accelerating action of heparin on the antithrombin III-inhibited activity of alpha-thrombin.

We have compared surface charge and the surface charge density on the polyanions heparin and potassium polyvinyl sulfate (KPVS), as well as on hydrolyzed heparin and KPVS, with their accelerating effect on the inhibitory action of antithrombin III on thrombin. Polyelectrolyte titration of thrombin with KPVS or heparin at pH 7.4 clearly indicates an electrostatic interaction. In contrast, at the same pH no electrostatic interaction is observed between polyanions and antithrombin III. KPVS accelerates the inhibitory action of antithrombin III to the same extent as heparin on the basis of charge equivalence. Heparin and KPVS with a mean distance between two charged centers of less than 0.75 and 0.95 nm, respectively, accelerate strongly whereas hydrolysates with lower charge densities are far less active. The following observations are indicated. Intramolecular neutralization of oppositely charged residues occurs within thrombin, antithrombin III, and partially hydrolyzed heparin. Heparin acts on the antithrombin III-thrombin reaction through cooperative electrostatic binding to thrombin and nonelectrostatic interaction with antithrombin III. This indicates a quasi-catalytic action of the polyelectrolyte. Hydrolysis of only a few N-sulfate residues within the heparin molecule decreases the linear surface charge density to such an extent that the accelerating action is drastically reduced. The loss of accelerating capacity agrees with the sudden loss of counterion condensation due to the decrease of the linear surface charge density beyond limits postulated by Manning in a theory of polyelectrolytes.

Antithrombin III↗