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PubMed2002

The distribution of counterions around synthetic rod-like polyelectrolytes in solution: a study by small-angle X-ray scattering and by anomalous small-angle X-ray scattering.

An investigation of the radial distribution of the counterions of a synthetic rodlike polyelectrolyte in aqueous solution is presented. The cationic polyelectrolyte used here has a poly(p-phenylene) backbone. For typical molecular weights the macroion comprises approximately one persistence length (ca. 20 nm) and effects of finite stiffness may be disregarded. Each repeating unit bears four charges which leads to a charge parameter of xi = 6.65. The distribution of the iodide counterions around this highly charged macroion is studied by small-angle X-ray scattering (SAXS) in dilute aqueous solution. These investigations are supplemented by measurements using anomalous small-angle X-ray scattering (ASAXS) that furnishes additional information about the contrast of the macroion. Data taken at high scattering angles give indication for contributions caused by the longitudinal fluctuations of the counterions. After correction for this effect the experimental results are compared to intensities calculated by use of the Poisson-Boltzmann (PB)-cell model. It is found that the PB-cell model describes the corrected data at intermediate and high scattering angles. Deviations at low scattering angle are attributed to the mutual interaction of the rod-like polyelectrolyte that can be described in terms of an effective structure factor. Data taken at lowest scattering angles point to a weak attraction between the rod-like macroions.

Journal Article↗
PubMed2002

Swelling of cross-linked polyelectrolyte gels.

A model of a cross-linked polyelectrolyte gel has been examined using Monte Carlo simulations. The simple model contained a charged defect-free network represented by linked charged beads and explicit counterions. Pressure-density relations for the polyelectrolyte gel, a corresponding non-ionic polymer gel, and several partly or fully degraded gels have been determined. The polyelectrolyte gel displayed a very large swelling capacity, in agreement with experiments. The swelling mechanism and chain properties are discussed and foundations of current theories on gel swelling are examined.

Journal Article↗
PubMed2002

Radial distribution function of rod-like polyelectrolytes.

We study the effect of electrostatic interactions on the distribution function of the end-to-end distance of a single polyelectrolyte chain in the rod-like limit. The extent to which the radial distribution function of a polyelectrolyte is reproduced by that of a wormlike chain with an adjusted effective persistence length is investigated. Strong evidence is found for a universal scaling formula connecting the effective persistence length of a polyelectrolyte with the strength of the electrostatic interaction and the Debye screening length.

Journal Article↗
PubMed2006

Mechanical property of lipid-coated polyelectrolyte microcapsules.

The deformations of lipid coated polyelectrolyte capsules induced by osmotic pressure were determined in poly(styrene sulfonate, sodium salt) (PSS) solution by making use of the fact that PSS molecules with a molecular weight 70000 will not penetrate into the capsules. At a critical osmotic pressure the initial spherical capsules changed their shape and became an invagination. The measurements of single particle light scattering provided the wall thickness of the lipid-coated capsules with 25.6 nm while the thickness for pure polyelectrolyte capsules in solution is about 21.6 nm, indicating that the coating lipid layer has about 4 nm thickness. It demonstrates that DMPA forms a bilayer on the surface of polyelectrolyte capsules. With these data, that the elasticity coefficient of the lipid-coated capsules is about 426 Mpa can be obtained.

Adsorption↗
PubMed2004

Frontal analysis continuous capillary electrophoresis for protein-polyelectrolyte binding studies.

A novel technique, frontal analysis continuous capillary electrophoresis (FACCE), has been described as an effective way to study protein-polyelectrolyte binding. FACCE involves continuous sampling, integrating sample injection and separation into one process that provides advantages over conventional frontal chromatography. The method provides rapid and precise determination of binding isotherms, and allows for quantitative binding analysis in terms of binding constant and the binding-site size by considering the protein as the ligand and allowing the polyelectrolyte to bind to a number of proteins with variable levels of cooperativity. FACCE is particularly suitable for binding systems involving rapid binding kinetics because it allows for the determination of the concentrations of free or bound ligands under conditions that avoid perturbation of the binding equilibrium. This chapter focuses on studies of the binding of bovine serum albumin (BSA) to heparin using FACCE. These investigations are demonstrated within the context of this chapter as representative of a model protein-polyelectrolyte system from which extensions to other systems can be made.

Animals↗
PubMed2003

Intelligent polyelectrolytes and gels in oral drug delivery.

The present review concerns smart, or intelligent polymers for oral administration that change conformation in aqueous solutions in response to external stimuli such as pH or temperature. We concentrate on charged polymers and gels with polyelectrolyte properties. Because of the ionization at a certain pH or in response to changes in the ionic composition of the solution, a polyelectrolyte has better chances of displaying smart properties than a neutral polymer. When such smart polyelectrolyte is cross-linked by covalent or hydrogen bonding and/or physical aggregation or is entangled, it forms an environmentally sensitive gel capable of swelling and collapse in an aqueous medium. Varying pH, temperature, and microbial flora are found in the gastrointestinal tract, and thus pH- sensitive polymers and gels that can be degraded by specific enzymes and/or inhibit proteolytic enzymes can be tailored for the efficient site-specific therapy. Smart polymers wield a lot of promise in the targeted, site-specific administration where they can provide advantages in loading of sensitive drugs such as proteins and peptides, while releasing the drug at a specific pH or in response to the presence of certain microbial flora.

Administration, Oral↗
PubMed2001

Flotation with polyelectrolytes as a first step of a more sustainable wastewater treatment system.

Within the framework of a research programme into more sustainable wastewater treatment systems based on physical-chemical pretreatment the application of dissolved air flotation (DAF) with polyelectrolytes as a primary treatment was investigated. Experiments with municipal wastewater were carried out in 2.5 I flotation batches and in a 100 I DAF pilot reactor. Two cationic polyelectrolytes (PEs) with molecular weights of 4 x 10(6) g/mol and 8 x 10(6) g/mol, were tested. The higher weight PE was more effective in removing turbidity and was used in the pilot experiments for coagulation/flocculation. Within the pilot system experiments the dry solids concentration of the float layer as well as the removal efficiencies of turbidity, CODparticulate, CODdissolved and nutrients, were studied. Typical results were that the obtained dry solids concentration of the floated sludge was 10%, when the float layer was removed after several hours. By using polyelectrolytes it was possible to remove more than 80% of CODparticulate and turbidity at dosages of 7-8 mg/g influent COD (i.e. 5 mg PE/100 NTU). The removal efficiency of CODdissolved was low. There was a proportional relationship between CODparticulate and turbidity. This led to the conclusions that by introducing a dosing control strategy based on continuous turbidity measurements a constant CODparticulate removal efficiency can be obtained.

Air↗
PubMed2002

Metallosupramolecular coordination polyelectrolytes: potential building blocks for molecular-based devices.

Metal-ion-induced self-assembly of ditopic ligands, based on bisterpyridines, and transition metal ions result in formation of metallosupramolecular coordination polyelectrolytes (MEPE). The positive charge of MEPE can be utilized in several ways to process highly ordered architectures. Alternating adsorption of MEPE and oppositely charged polyelectrolytes on solid substrates results in multilayers. The sequential nature of this process allows combining MEPEs with other functional components. This process permits nanometer thickness control, is readily adapted for automated processing, and is applicable to two-dimensional substrates as well as to colloidal templates. The surface chemical properties of MEPE are readily controlled by complexing MEPE with negatively charged amphiphiles. The resulting polyelectrolyte-amphiphile complexes (PAC) are soluble in organic solvents and form liquid crystalline phases. The PAC also spreads at the air-water interface as Langmuir monolayer, which can be transferred onto solid substrates. The resulting Langmuir-Blodgett multilayers are highly ordered and anisotropic. Materials with transition metal ions possess many interesting properties, including spin transitions, magnetism, as well as photochemical assets that are relevant for the construction of functional devices and materials. The presented approach combines principles of supramolecular and colloidal chemistry as well as surface science, is highly modular in nature, and provides extensive control of structure and function from molecular to macroscopic levels.

Air↗
PubMed2006

Decellularized umbilical artery treated with thin polyelectrolyte multilayer films: potential use in vascular engineering.

Decellularized allograft tissues have been identified as a potential extracellular matrix scaffold for tissue-engineered vascular substitutes. In order to improve the thromboresistance, it is necessary to pre-coat the intra-luminal vessel surface. Recently a new surface modification technique appeared, based on the alternate adsorption of positive and negative charged polyelectrolytes. Our objective was to develop an alternative vascular scaffold made of decellularized human umbilical arteries treated with a PAH/PSS polyelectrolyte multilayered film. The vessels luminal surfaces covered with the multilayer film were observed by electronic scanning microscopy. Our observations showed that the luminal surface is completely devoid of ECs following treatment with trypsin. A top view of the coated artery indicated that the multilayer uniformly covered internal surface of the vessels. The successful of the multilayer correct deposition and retention on the arterial wall were controlled by confocal microscopy using a fluorescent polyelectrolyte (rhodamine-PAH). The data suggest that decellularized cryopreserved arteries represent a potential scaffold for further vascular tissue engineering efforts. Moreover, the multilayer films can be used to coat biological surfaces and following the terminated layer (PAH or PSS), favour the cell adhesion or cell resistance.

Arteries↗
PubMed1985

Persistence of staphylococcal cell-wall components in inflammatory sites may be due to the modulation by sulphated polyelectrolytes of autolytic wall enzymes: a working hypothesis.

The interaction of leucocytes with Staphylococcus aureus results in killing of the bacterial cells, but large portions of the bacterial cell walls persist apparently phagocytic cells for long periods. The mechanisms of biodegradation of staphylococci by leucocyte factors have shown that degradation of cell walls in vitro may be the result of the activation, by leucocyte kationic proteins, of the bacterial autolytic wall enzymes that are responsible for degrading the cell walls from within. This process is markedly inhibited by sulphated polysaccharides like dextran sulphate, by heparin, or by polyanetholesulfonate (liquoid). These anionic polyelectrolytes have also been shown to inhibit the lysis of staphylococci treated with bacteriolytic concentrations of penicillin G. Staphylococci injected intraarticularly into the knee joint of rats underwent massive plasmolysis, but structures compatible with cell walls (peptidoglycan) persisted within macrophages in the inflammatory sites, for long periods. It is postulated that the inability of leucocytes to degrade staphylococcal cell-wall components may be the result of the interference, by anionic polyelectrolytes likely to accumulate in the inflammatory sites, with the activation of the autolytic systems. Alternatively, anionic polyelectrolytes may coat the bacterial cells and interfere with the binding of the autolytic enzymes with their corresponding substrates.

Animals↗
PubMed1981

[Modification of the immune response by using an antigen bound to synthetic polyelectrolytes].

The immunogenic properties of the soluble complexes of bovine serum albumin (BSA) and synthetic polyelectrolytes were studied. The polyelectrolytes used in these complexes were 4-vinyl-N-ethylpyridinium bromide and 4-vinyl-N-cetylpyridinium bromide (complex I), 4-vinylpyridine and 4-vinyl-N-acetylpyridinium bromide (complex II). C57BL mice were immunized with different doses of BSA, complexes I and II introduced intraperitoneally in a single injection, and the number of plaque-forming cells (PFC) in the spleen was determined by modified Jerne's test with the use of BSA-covered sheep red blood cells. The above complexes were shown to stimulate the production of PFC against BSA 50-100 times more intensively than pure BSA. The mixtures of BSA with the above-mentioned polyelectrolytes stimulated PFC production to a considerably lesser extent. Thus, the polymeric part of these conjugates was not an antigen, but served as a carrier inducing pronounced immune response to the antigenic (protein) part of the complex.¿¿¿¿¿¿¿¿¿¿¿¿¿¿¿¿¿¿¿¿¿¿¿¿¿¿¿¿¿¿

Animals↗
PubMedDate not supplied

[Calculation of the intrinsic viscosity of synthetic and biological polyelectrolytes of various rigidity].

On the basis of the excluded-volume effect theory for nonionic polymer molecules developed by Alexandrowicz semi-empirical formulas for calculation of the intrinsic viscosity [eta] of polyelectrolytes of various rigidity are proposed. The expression for the second virial coefficient of gas consisting of cylindrical particles is used for the determination of explicit form of the effective excluded volume of the segment upsilon0. In addition the alteration of Flory's parameter phi (epsilon) by the expansion of a macromolecule, and the alteration of thermodynamic rigidity A of the polyelectrolyte molecule in the range of low ionic strengths mu have been taken into account. All that leads to good agreement between calculated and experimental values of [eta] of polyelectrolytes under consideration, i. e. native and denatured DNA and poly (acrylic acid), in a wide range of mu. The calculated dependence A = A (mu) providing the best agreement between the theoretical and experimental values of [eta], also describes reasonably the experimental dependence A = A (mu) obtained from the macromolecule's optical anisotropy measurements for native DNA or from unperturbed dimensions of the macromolecule, determined on the basis of the Stockmayer and Fixman equation for denatured DNA.

Biopolymers↗
PubMed2004

Zeta potential as a measure of polyelectrolyte flocculation and the effect of polymer dosing conditions on cell removal from fermentation broth.

Characterization of flocculation for cell removal from fermentation broth via polyelectrolyte addition is commonly based on qualitative methods such as physical appearance of the floc. The use of zeta potential as a quantitative measure of floc character was evaluated as an indicator of optimal polymer addition. Zeta potential was found to increase with increasing cationic polyelectrolyte dosage, but never reached zero regardless of the total amount of polymer added, indicating flocculation occurs at least partially through a bridging type mechanism. Experiments were conducted using various polymer concentrations (25-75 g/L) and dosing methods (batch, incremental and continuous addition) that resulted in variable overall polymer requirements to achieve optimum flocculation. Zeta potential was found to be constant at optimal floc character regardless of the total amount of polymer added, polymer concentration, or method of polymer addition. Experiments with two additional types of fermentation broth also showed characteristic zeta potentials at optimal flocculation. Polymer requirements to achieve a particular floc character can vary greatly, depending on polymer dosing conditions and fermentation batch. The effect of polymer dosing conditions on the polymer requirement to obtain optimal floc character was evaluated. Polymer dosing method and calcium concentration were both found to have a significant effect (P < 0.0001) with continuous polymer addition and high calcium concentration requiring less polymer than did batch polymer addition and low calcium concentration, respectively. Polymer dosing concentration did not significantly affect polymer requirement for optimal flocculation.

Bacillus↗
PubMed2001

Determination of protection from serum nuclease activity by DNA-polyelectrolyte complexes using an electrophoretic method.

Polyelectrolyte complexes between cationic polymers and DNA have emerged as potential nonviral vectors for DNA delivery. For successful in vivo delivery, methods for analyzing their ability to prevent digestion of the DNA payload by serum nucleases are essential. We report here a simple assay to determine degradation of DNA in these complexes using standard electrophoretic techniques. The assay is based on a high pH buffer which can dissociate the complexes under standard electrophoretic conditions. This assay can be used qualitatively to determine the time taken for degradation to occur. Alternatively, with a standard gel analysis program it can be used quantitatively to investigate rates of DNA degradation from complexes in the presence of serum nucleases. We have shown that it can distinguish between different formulations with the same polymer, and also to distinguish between the time taken to degradation and the rates of degradation of DNA in complexes formed with two structurally related, linear polyamidoamine polymers. The assay could also distinguish between the time to degradation using poly-l-lysine complexes, although these were less well dissociated by the electrophoresis buffer, and could not be analyzed quantitatively. This assay will be of value in investigating and developing polyelectrolyte formulations for parenteral administration.

Buffers↗
PubMed2005

Effect of functionalization of multilayered polyelectrolyte films on motoneuron growth.

We studied in vitro cell-substrate interaction of motoneurons with functionalized polylectrolyte films. Thin polylectrolyte films were built on glass by alternating polycations, poly(ethylene-imine) PEI, poly(L-lysine) PLL, or poly(allylamine hydrochloride) PAH, and polyanions, poly(sodium-4-styrenesulfonate) PSS or poly(L-glutamic acid) (PGA). These architectures were functionalized with Brain Derived Neurotrophic Factor (BDNF) or Semaphorin 3A (Sema3A). We used Optical Waveguide Lightmode Spectroscopy (OWLS) and Atomic Force Microscopy (AFM) to characterize the architectures. The viability of motoneurons was estimated by the acid phosphatase method, and morphometrical measures were performed to analyse the influence of different architectures on cell morphology. Motoneurons appeared to adhere and spread on all the architectures tested and preferentially on PSS ending films. The viability of motoneurons on polyelectrolyte multilayers was higher compared to polyelectrolyte monolayers. BDNF and Sema3A embedded in the films remained active and thereby create functionalized nanofilms.

Animals↗
PubMed2005

Natural polyelectrolyte films based on layer-by layer deposition of collagen and hyaluronic acid.

The aim of the present work was to assemble extracellular matrix components into polyelectrolyte multilayers using the layer-by-layer deposition method. The films are constructed with type-I collagen and hyaluronic acid. The construction exhibits the general features observed during polyelectrolyte multilayer buildup: alternate positive and negative values of the zeta potential of the film during its construction and regular increase of the film thickness with the number, n, of deposition step. This increase is shown to be linear with n. As expected for a linearly growing film, the confocal microscopy shows that when the film is brought in contact with a collagen solution, collagen does not diffuse into the film but interacts only with its outer layer. However, the films are not constituted of homogeneously distributed polyanion/polycation complexes as it is usually observed, but they are formed of fibers as imaged by AFM. The typical width of these fibers increases with the number of deposition steps. Finally, it is found that chondrosarcoma cells spread well and synthesize extracellular matrix components only on the collagen ending films, whereas no cellular matrix was found for HA ending ones. Such architectures may be further functionalized by inclusion of active drugs, peptides, proteins..., and could be used as tunable biomaterial interfaces.

Biocompatible Materials↗
PubMed2005

Biologically active lipid A antagonist embedded in a multilayered polyelectrolyte architecture.

Recently [Jessel N, Schwinte P, Donohue R, Lavalle P, Boulmedais F, Darcy R, et al. Pyridylamino-beta-cyclodextrin as a molecular chaperone for lipopolysaccharide embedded in a multilayered polyelectrolyte architecture. Adv Funct Mater 2004;14:963-9], we demonstrated the biological activity of a lipopolysaccharide from Escherichia coli incorporated into layer-by-layer films made of poly (l-lysine) and poly (l-glutamic acid) and containing a polycationic beta-cyclodextrin (CD) with chaperone properties. Here we develop innovative architectures containing a complex made of a charged beta-cyclodextrin and a lipid A antagonist (LAA) as potential systems for local endotoxin antagonistic activity. We examine the biological activity of these architectures. The CD-LAA complex adsorbed on top, or embedded into the polyelectrolyte films keeps its LPS antagonistic activity on both murine and human macrophages for at least 24h.

Animals↗
PubMedDate not supplied

Permeation of macromolecules into polyelectrolyte microcapsules.

Polyelectrolyte microcapsules (PEMCs) have been prepared by coating red blood cells with the polyelectrolytes poly(styrenesulfonate), poly(allylamine hydrochloride), and dextran sulfate applying the layer-by-layer technique with subsequent dissolution of the core. The capsule permeability for human serum albumin (HSA) was studied as a function of the ionic strength and pH by means of confocal microscopy. PEMCs produced with dextran sulfate and poly(allylamine hydrochloride) show a significant increase in permeability for HSA at salt concentrations over 1 mM. For PEMCs prepared with poly(styrenesulfonate) and poly(allylamine hydrochloride) the limiting salt concentration is 5 mM. No pH dependence for permeation was observed. A correlation between the permeation and adsorption of HSA on the PEMC walls was investigated. Finally, a mechanism for the permeability, combining electrostatic interactions, and the presence of pores in the polymer layers is presented confirmed by the considerable increase of permeation of charged molecules in the presence of salt and the permeation of neutral molecules regardless of the ionic strength.

Biopolymers↗