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PubMedDate not supplied

Polyelectrolyte complexes and layer-by-layer capsules from chitosan/chitosan sulfate.

Polyelectrolyte complex formation of chitosans of varying average molecular weight and degree of acetylation with chitosan sulfate or poly(styrene sulfonate) was studied by static light scattering in dilute solution at various ionic strengths. Unlike the molecular weight, the degree of acetylation was found to have a significant effect on the resultant structural densities of the complexes. The same system was applied to the preparation of micrometer-sized hollow shells by means of a layer-by-layer technique (in total eight layers). Their behavior toward fluorescent probes such as fluorescein and rhodamin 6G or fluorescein isothiocyanate labeled dextrans at various ionic strengths and pH (observed by confocal laser light scanning microscopy) could be understood through a discussion of electrostatic forces between the highly charged shells and the probes to be dominant. At an ionic strength of 0.1 M and above, charge effects are largely suppressed (screening effect) and a size-dependent "cutoff" for the permeation of the macromolecular fluorophore was observed.

Acetylation↗
PubMed2004

Fabrication of composite films containing zirconia and cationic polyelectrolytes.

Composite films were prepared by electrophoretic deposition of poly(ethylenimine) or poly(allylamine hydrochloride) combined with cathodic precipitation of zirconia. Films of up to several micrometers thick were obtained on Ni, Pt, stainless-steel, graphite, and carbon-felt substrates. When the concentration of polyelectrolytes in solutions and the deposition time were varied, the amount of the deposited material and its composition can be varied. The electrochemical intercalation of yttria-stabilized zirconia particles into the composite films has been demonstrated. Obtained results pave the way for the electrodeposition of other polymer-ceramic composites. The deposits were studied by thermogravimetric analysis, X-ray diffraction analysis, scanning electron microscopy, and atomic force microscopy. The mechanisms of deposition are discussed.

Polyamines↗
PubMed2004

Micropatterning neuronal cells on polyelectrolyte multilayers.

This paper describes an approach to adhere retinal cells on micropatterned polyelectrolyte multilayer (PEM) lines adsorbed on poly(dimethylsiloxane) (PDMS) surfaces using microfluidic networks. PEMs were patterned on flat, oxidized PDMS surfaces by sequentially flowing polyions through a microchannel network that was placed in contact with the PDMS surface. Polyethyleneimine (PEI) and poly(allylamine hydrochloride) (PAH) were the polyions used as the top layer cellular adhesion material. The microfluidic network was lifted off after the patterning was completed and retinal cells were seeded on the PEM/PDMS surfaces. The traditional practice of using blocking agents to prevent the adhesion of cells on unpatterned areas was avoided by allowing the PDMS surface to return to its uncharged state after the patterning was completed. The adhesion of rat retinal cells on the patterned PEMs was observed 5 h after seeding. Cell viability and morphology on the patterned PEMs were assayed. These materials proved to be nontoxic to the cells used in this study regardless of the number of stacked PEM layers. Phalloidin staining of the cytoskeleton revealed no apparent morphological differences in retinal cells compared with those plated on polystyrene or the larger regions of PEI and PAH; however, cells were relatively more elongated when cultured on the PEM lines. Cell-to-cell communication between cells on adjacent PEM lines was observed as interconnecting tubes containing actin that were a few hundred nanometers in diameter and up to 55 microm in length. This approach provides a simple, fast, and inexpensive method of patterning cells onto micrometer-scale features.

Animals↗
PubMedDate not supplied

A two-step process for controlling the surface smoothness of polyelectrolyte-based microcapsules.

Biocompatibility is one of the crucial requirements to be fulfilled when designing devices for immunoisolation of transplanted cells. The quality of the capsule surface (smoothness/roughness) influences the nature of cell overgrowth on it by immunocytes, which eventually may lead to the transplant failure. A microcapsule has been developed based on the polyelectrolyte complexation of the polyanions sodium alginate and cellulose sulphate with the polycation poly(methylene-co-guanidine), which was successfully tested in rodent animal models. Recently, the principles for controlling the surface smoothness of these capsules has been identified. This paper reports on a two-step process used for production of stable capsules with improved surface properties. The methodology involves separating the process of drop shape recovery and precursor capsule formation from the process of membrane formation by applying a two-reactor design. The multi-loop reactors are connected in series, and the process separation is given by the different composition of cation solutions flowing in each reactor. This process enables one to prepare the microcapsule immunoisolation device, which can differ in the extent of surface roughness and, thus, is suitable for studying the effect of surface morphology of the immunoisolation device on cell overgrowth. The effect of this process on the capsule permeability has also been evaluated.

Alginates↗
PubMed2005

Rapid polyelectrolyte-based membrane immunoassay for the herbicide butachlor.

Oppositely charged water-soluble polyelectrolytes were used in the developed membrane immunoenzyme assay for the herbicide butachlor. High-affinity and rapid binding between polyanion polymethacrylate and polycation poly(N-ethyl-4-vinylpyridinium) was applied to separate reacted and free immunoreactants. Competitive immunoassay format with peroxidase-labeled antigen was realized. The insoluble colored product of the peroxidase reaction was formed by bound labeled immune complexes and was reflectometrically detected. The assay combines short duration (15 min), high sensitivity (0.03 g/mL) and availability for out-of-laboratory testing. Different image processing algorithms were used to determine the herbicide content. Low variation coefficients of the measurements in the proposed quantitative assay, namely 4.8-9.0% for the range of antigen concentrations from 0.1 to 3.0 ng/mL, are evidence of the assay effectiveness. Possibility to control the butachlor content in mineral, artesian, and drinking water was demonstrated.

Acetanilides↗
PubMed1999

Buckling, fluctuations, and collapse in semiflexible polyelectrolytes.

We present a systematic statistical mechanical analysis of the conformational properties of a stiff polyelectrolyte chain with intrachain attractions that are due to counterion correlations. We show that the mean-field solution corresponds to an Euler-like buckling instability. The effect of the conformational fluctuations on the buckling instability is investigated, first, qualitatively, within the harmonic ("semiclassical") theory, then, systematically, within a 1/d expansion, where d denotes the dimension of embedding space. Within the "semiclassical" approximation, we predict that the effect of fluctuations is to renormalize the effective persistence length to smaller values, but not to change the nature of the mean-field (i.e., buckling) behavior. Based on the 1/d expansion we are, however, led to conclude that thermal fluctuations are responsible for a change of the buckling behavior which is turned into a polymer collapse. A phase diagram is constructed in which a sequence of collapse transitions terminates at a buckling instability that occurs at a place that varies with the magnitude of the bare persistence length of the polymer chain, as well as with the strength and range of the attractive potential.

Chromosome Structures↗
PubMed1986

[Isolation and properties of prostaglandin H synthetase immobilized in insoluble polyelectrolyte complexes].

Immobilization of prostaglandin-H-synthetase (EC 1.14.99.1) of the microsomal fraction of ram vesicular gland in the microparticles of insoluble polyelectrolyte complexes by non-covalent incorporation was studied. It was shown that immobilization occurs with a high efficiency and high activity yield (40-70%). Non-specific reversible inhibition of the enzyme by the polycationic component of the complex was demonstrated. The dependencies of activity of the native and immobilized enzymes on pH, temperature and substrate (adrenaline and arachidonic acid) were studied. The immobilized enzyme had an increased thermal stability as compared to the native one; the thermoinactivation rate constant was decreased 3-7 times. The biexponential type of the curve of the rependence of activity vs. time for the native enzyme and the transformation of the curve into a simple exponential form for the immobilized enzyme were observed.

Animals↗
PubMed1996

Polarization of counterions in polyelectrolytes.

A theory of the polarization of counterions bound to a polyion, such as a DNA, in low and high electric field strengths is developed using statistical mechanics of inhomogeneous systems. For low fields, one finds that the polarizability p is (Zq)2rho0betaL3/(12[l + Lrho0sigma(L, b, xi, Z, I, rho0)]), where sigma = integral1 0(lambda' - lambda0) ¿dc(lambda - lambda')/dlambda¿lambda = lambda0 dlambda']), Z and L are the valence and the length of the polyion, respectively, q is the proton charge, beta = 1/kBT, T is the temperature, kB is the Boltzmann constant, I is the ionic strength, lambda = x/L and lambda0 = x0/L are scaled distances, x0 is a reference point such that the inhomogeneous counterion density at x0 is equal to rho0--the uniform density in the absence of an electric field E--and c(x) is the direct correlation function of the homogeneous counterion-polyion phase, which includes attractive and repulsive interactions. If Lsigma(L, ...) is much less than one, then the polarizability is proportional to L3. If the term Lsigma(L, ...) is much larger than one, the polarizability scales as L2. The induced dipole moment saturates and its value is the same as that of Mandel-Manning theories. The onset of the saturation, however, depends critically on the direct correlation function and hence polyelectrolyte effects. In the formalism, the polarization of the counterions is the equilibrium response to an electric field provided E is less than Esaturated. A dynamical scheme that incorporates the fact that in high fields the bound counterions conduct is discussed.

Chemical Phenomena↗
PubMed1998

Effects of polyelectrolyte complex (PEC) on human periodontal ligament fibroblast (HPLF) function. I. Three-dimensional structure of HPLF cultured on PEC.

Human periodontal ligament fibroblast (HPLF) cultured on tissue culture dishes (TCD), irrespective of the presence of serum, showed only a spreading form. In contrast, using polyelectrolyte complex (PEC) as a matrix, HPLF showed spreading, round, and aggregate forms. Cells of the inner part of the aggregate contacted with each other to form a three-dimensional structure, and this condition corresponded to typical tissues in vivo. These seemed to be related to the interrelation between growth and morphology; that is, the HPLF of the spreading form was considered to belong to a proliferation phase, and the HPLF of the round and aggregate forms, with a little growth, seemed to belong to a functional phase of the cell cycle, indicating that PEC is able to control such cell functions as proliferation, morphology, and differentiation. The cell aggregate was observed only on PEC with carboxymethyl residues and was stained by alizarin red (AR), which suggested mineralization. The spreading cells on PEC containing sulfate residues were not stained by AR. Therefore, it was found that there was a certain relationship between cell growth and morphology, and that PEC affected the cell cycle and promoted proliferation and differentiation of HPLF.

Biocompatible Materials↗
PubMed1998

Effects of polyelectrolyte complex (PEC) on human periodontal ligament fibroblast (HPLF) function. II. Enhancement of HPLF differentiation and aggregation on PEC by L-ascorbic acid and dexamethasone.

In addition to many types of extra cellular matrix (ECM) in vivo, cells are stimulated by many types of vitamins, hormones, growth factors, etc. In this paper the effects of L-ascorbic acid 2-phosphate (Asc-2P) and dexamethasone (Dex) on proliferation and differentiation of human periodontal ligament fibroblast (HPLF) using polyelectrolyte complex (PEC) as a matrix in vitro will be discussed. The PEC was composed of chitosan as a polycation, with carboxymethyl (CPEC) or sulfated chitin (SPEC). Asc-2P (0.2 mM) inhibited the growth of HPLF on CPEC, but promoted the growth on SPEC. Moreover, the aggregation of HPLF on CPEC was inhibited by Asc-2P, but that on SPEC was induced in the presence of Asc-2P and Dex. Although Asc-2P reduced an increase in alkaline phosphatase (ALPase) activity of HPLF on CPEC as well, it induced a twofold increase in ALPase activities on SPEC and TCD. Furthermore, in the medium containing Asc-2P and 100 mM of Dex, cell growth was inhibited, but ALPase activity was promoted on both SPEC and TCD to form many aggregates on SPEC. ALPase activity increased by twofold over that of HPLF cultured in the medium containing only Asc-2P. Therefore, it is suggested that the cell functions of HPLF are controlled by the combination of PEC and additives.

Alkaline Phosphatase↗
PubMed1998

Reactivation of glyceraldehyde-3-phosphate dehydrogenase using conjugates of monoclonal antibodies with polyelectrolyte complexes. An attempt to make an artificial chaperone.

The simplified model of chaperone action when the inactive misfolded forms are removed from the reaction media preventing aggregation was developed using antibodies in combination with polyelectrolyte complexes. The antibodies, which bind specifically inactive dimers of glyceraldehyde-3-phosphate dehydrogenase but not native tetramers, were coupled covalently to poly(methacrylic acid). The treatment of inactivated GAPDH with this conjugate followed by its precipitation after equimolar addition of polycation, poly-(N-ethyl-4-vinylpyridinium bromide), resulted in a significant increase in the specific activity of the enzyme.

Animals↗
PubMed1999

Controllable stability of DNA-containing polyelectrolyte complexes in water-salt solutions.

Destruction of polyelectrolyte complexes (PECs) formed by DNA and synthetic polyamines of different structures was carried out by addition of low molecular weight electrolyte to PEC solution at different pHs. The dissociation was studied by the fluorescence quenching technique using the ability of cationic dye ethidium bromide to intercalate into free sites of DNA double helix followed by ignition of ethidium fluorescence. Structure of amine groups of the polycation was shown to be a decisive factor of PEC stability. PECs formed by polycations with quaternary amine groups, i.e., poly(N-alkyl-4-vinylpyridinium) bromides, poly(N, N-dimethyldiallylammonium) chloride, and ionene bromide, were pH independent and the least tolerant to destruction by the added salt. Primary amine groups of basic polypeptides poly-L-lysine hydrobromide and poly-L-arginine hydrochloride as well as synthetic polycation poly(vinyl-2-aminoethyl ether) provided the best stability of PECs in water-salt solutions under wide pH range. Moderate and pH-dependent stability was revealed for PECs included poly(N,N-dimethylaminoethylmethacrylate) with tertiary amine groups in the chain or branched poly(ethylenimine) with primary, secondary, and tertiary amine groups in the molecule. The data obtained appear to be the basis for design of DNA-containing PECs with given and controllable stability. The design may be accomplished not only by proper choice of polyamine of one or another type, but by using of tailor-made polycations with given composition of amine groups of different structure in the chain as well. Thus, quaternization of a part of tertiary amine groups of poly(N, N-dimethylaminoethylmethacrylate) resulted in expected decrease of stability of DNA-containing PECs in water-salt solutions. The destruction of PEC formed by random copolymer of 4-vinylpyridine and N-ethyl-4-vinylpyridinium bromide was pH sensitive and could be performed under pH and ionic strength closed to the physiological conditions. This result appears to be particularly promising for addressing DNA packed in PEC species to the target cell.

DNA↗
PubMed2001

On the use of the activation energy concept to investigate analyte and network deformations in entangled polymer solution capillary electrophoresis of synthetic polyelectrolytes.

The activation energy associated with the electrophoretic migration of an analyte under given electrolyte conditions can be accessed through the determination of the analyte electrophoretic mobility at various temperatures. In the case of the electrophoretic separation of polyelectrolytes in the presence of an entangled polymer network, activation energy can be regarded as the energy needed by the analyte to overcome the obstacles created by the separating network. Any deformation undergone by the analyte or the network is expected to induce a decrease in the activation energy. In this work, the electrophoretic mobilities of poly(styrenesulfonates) (PSSs) of various molecular weights (Mr 16 x 10(3) to 990 x 10(3)) were determined in entangled polyethylene oxide (PEO) solutions as a function of temperature (in the 17-60 degrees C range) and the PSS activation energies were calculated. The influences of the PSS molecular weight, blob sizes zetab of the separating network (related to the PEO concentration), ionic strength of the electrolyte and electric field strength (75-600 V/cm) were investigated. The results were interpreted in terms of analyte and network deformations and were confronted with those previously obtained for DNA migration in polymer solutions and chemical gels. For a radius of gyration Rg zetab, suggesting PSS and network deformations in the latter case. Increasing ionic strength resulted in an increase in the PSS activation energy, because of the decrease of their radii of gyration, which makes them less deformable. Finally, the activation energies of all the PSSs are a decreasing function of field strength and at high field strength tend to reach a constant value close to that for a small molecule.

DNA↗
PubMed2004

Tailor-made polyelectrolyte microcapsules: from multilayers to smart containers.

This review addresses the fabrication and properties of novel polyelectrolyte microcapsules, with an emphasis on their mechanical and permeability properties. Ease of preparation through layer-by-layer self assembly, accurate control over wall thickness as well as flexibility in the choice of constituents make these capsules very promising for numerous applications in materials and life science. Moreover, by engineering the inner and outer interfaces, these capsules can be used as microreactors for precipitation, crystallization, and polymerization reactions, as well as enzymatic, and heterogeneous catalysis.

Biocompatible Materials↗
PubMed2005

Novel polyelectrolyte carboxymethyl konjac glucomannan-chitosan nanoparticles for drug delivery. I. Physicochemical characterization of the carboxymethyl konjac glucomannan-chitosan nanoparticles.

Carboxymethyl konjac glucomannan-chitosan (CKGM-CS) nanoparticles, which are well dispersed and stable in aqueous solution, were spontaneously prepared under very mild conditions via polyelectrolyte complexation. The physicochemical properties of the nanoparticles were identified by Zetasizer 3000 and Fourier transform infrared. It was found that at various CKGM and CS concentrations the particles ranged in size from approximately 50 to 1200 nm, and the zeta potential from 15 to 45 mV. By changing pH value of the medium and increasing the concentration of salt, the mean size of the particles increased and the zeta potential decreased. Also, investigations on the encapsulation efficiency of the bovine serum albumin loaded CKGM-CS nanoparticles were also undertaken. This nanoparticulate system driven by complex formation shows potential as an advanced drug delivery system for water-soluble drugs.

Chitosan↗
PubMed1991

Polyelectrolyte properties of biopolymers: conductivity and secondary structure of polyriboadenylic acid and its salts in solutions.

Polyriboadenylates of alkali metals were obtained from (1) K(+)-poly(A) (salts 1) and (2) H(+)-poly(A) (salts II) by the ion-exchange method. The conductivity of these salts as well as of H(+)-poly(A) were studied. Salts I and II of the same counterion were shown to have significantly different conductivity coefficients (f) and polyion conductances (lambda 0p). the charge density parameter (xi) was 1.3 and 2.5, respectively, with lambda 0p equal to 44 and 83 ohm-1 cm2 mole-1 for poly(A)-I and poly(A)-II salts, respectively. This is credited to the difference in the conformations of corresponding polyions. The linear dependence of equivalent conductivity on the square root of polymer concentration (Kohlrausch coordinates), earlier obtained for DNA, is also satisfied for the studied polynucleotides. A comparison of the slopes of straight lines in Kohlrausch coordinates for poly(A), simple electrolytes, and for earlier studied polyribouridylic acid salts lends credence to the concepts, developed by a number of authors, that DNA can act as a "buffer" against the ion-ion interaction in concentrated electrolyte solutions. Using the approximation that the polyion conductance is independent of the counterion nature, parameter f (agreeing in this case with Eisenberg parameter phi) has been shown to decrease as the polynucleotide concentration is increased; the decrease is caused by the relaxation effect. The transference numbers of counterions, which have negative values in poly (A)-II solutions, grow with the increase in polymer concentration; the higher the xi, the more apparent is this increase. This is explained by the increase in the fraction of conductivity along the polyion chains ("surface" conductivity) with the growth of polyelectrolyte concentration.

Electric Conductivity↗
PubMed2003

Phospholipase A2 hydrolysis of mixed phospholipid vesicles formed on polyelectrolyte hollow capsules.

Mixtures of the phospholipids L-alpha-dimyristoylphosphatidic acid (DMPA) and L-alpha-dipalmitoylphosphatidylcholine (DPPC) have been successfully adsorbed onto the charged surface of multilayer polyelectrolyte capsules to form a novel vesicle. Leaving such vesicles in phospholipase A(2) solution, we observed the hydrolysis reaction on the surface of the lipid/polymer vesicles and a permeability change before and after the reaction by confocal-laser scanning microscopy (CLSM). A capsule with adjustable permeability was constructed. This method may provide new features for drug-release vesicles.

1,2-Dipalmitoylphosphatidylcholine↗
PubMed2003

Swelling and shrinking of polyelectrolyte microcapsules in response to changes in temperature and ionic strength.

Swelling and shrinking of polyelectrolyte microcapsules consisting of poly(styrene sulfonate, sodium salt) (PSS) and poly(diallyldimethyl ammonium) chloride (PDADMAC) multilayers have been observed in response to temperature and electrolyte exposure, respectively. Heat-induced capsule swelling and capsule wall volume reduction were observed by confocal laser scanning microscopy (CLSM) and scanning force microscopy (SFM). On the other hand, pronounced shrinking in diameter induced by exposure to an electrolyte was observed in parallel to increases in the thickness of the capsule wall. The estimated wall volume was reduced to two thirds of the control for the salt-exposed capsules and one half for the salt-exposed and simultaneously annealed capsules. This reduction in volume was supposedly mainly caused by the compression of the capsule wall due to the ionic screening from the electrolyte. The highly porous microstructure of the multilayers and loosely bound PSS/PDADMAC complex are thought to be responsible for the structure of the PSS/PDADMAC capsules being easily modulated upon annealing and salt-exposure.

Journal Article↗