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PubMed2004

AFM observation of collapse and expansion of phosphoric acid-demineralized dentin.

The objective of this study is to provide additional data regarding morphological changes that occur to dentin matrices following demineralization with etchants. Our understanding of the mechanism of diffusion of comonomers into the demineralized substrate is very limited. It has been hypothesized that certain water-soluble polyelectrolytes (acidic proteins) and neutral proteins in dentin can influence the collapse of demineralized dentin when it is air dried. Some of these solubilized substances are thought to aggregate by the action of Ca cations, which become dissolved during H(3)PO(4) etching, ultimately resulting in some degree of collapse. In the current study, dentin surfaces were examined by atomic force microscopy (AFM) before and after treatment by 10% H(3)PO(4)containing increasing concentrations of CaHPO(4). Reversal of matrix collapse by aqueous 30% 2-hydroxyethyl methacrylate (HEMA) was evaluated by AMF for 60 min. The results demonstrate two forms of matrix collapse; we speculate that one form is induced by acidic noncollagenous polyelectrolytes and the other by neutral peptides. Our data indicate that further evaluation of the influence of endogenous noncollagenous proteins must be studied to understand the mechanism of the collapse and reexpansion dynamics of demineralized dentin networks.

Animals↗
PubMed2004

Improved wet bonding of methyl methacrylate-tri-n-butylborane resin to dentin etched with ten percent phosphoric acid in the presence of ferric ions.

The objective of this study was to determine the influence of dissolved dentinal substances in demineralized dentin on the hybridization of resin for bonding to dentin. It was hypothesized that these substances, including polyelectrolytes, significantly change the substrates, which could then be assessed by the addition of Na(+), Ca(2+), or Fe(3+) in 10% phosphoric acid. Bovine dentin specimens were etched for 10 s with a solution of 10% phosphoric acid (control) or of 22.0 mM dissolved sodium chloride (10P-Na), calcium chloride (10P-Ca), or ferric chloride (10P-Fe). The specimens were then rinsed, blot-dried, and primed three times with 5% 4-methacryloyloxyethyl trimellitate anhydride in acetone for 60 s. Methyl methacrylate-tri-n-butylborane resin was then applied. The tensile bond strength of each of the dumbbell-shaped specimens was then measured. The fractured surfaces and modified cross-sections were examined by scanning electron microscopy. The cross-sections were soaked in 6N HCl for 10 s and then in 1% sodium hypochlorite for 30 min to determine the resin content in the hybridized specimens. Shrinkage of the demineralized dentins upon drying was assessed by atomic force microscopy. The tensile bond strengths were 10.8 +/- 4.5 (control), 15.0 +/- 7.0 (10P-Na), 19.3 +/- 5.5 (10P-Ca), and 27.8 +/- 8.1 (10P-Fe) MPa. The atomic force microscopy studies showed that Fe(3+) minimized the shrinkage by drying for 10 s but Ca(2+) and Na(+) did not decrease the shrinkage the same as the control. The results support the hypothesis that the monomer permeability of wet demineralized dentin is effectively improved by dissolving ferric ions in the phosphoric acid, resulting in a greater bond strength and higher resin content in the hybridized dentin. The dissolved dentinal substances, including the polyelectrolytes, had a significant influence on the characteristics of the demineralized dentin, changing the degree of hybridization and bonding.

Animals↗
PubMed2004

Encapsulation of biologics in self-assembled fibers as biostructural units for tissue engineering.

The concept of a "biostructural unit" is presented as the combination of biological and structural building blocks to create scaffolds or constructs via a bottom-up approach. Three types of biostructural units were constructed using the process of fiber formation by interfacial polyelectrolyte complexation: protein-encapsulated fiber, ligand-immobilized fiber, and cell-encapsulated fiber units. Water-soluble chitin (WSC) and alginate were used as the polyelectrolyte combination to form fiber. Encapsulation and sustained release of bovine serum albumin from the fiber could be achieved, release profiles being dependent on the WSC/alginate concentration ratio. Released nerve growth factor (NGF) retained its bioactivity, as demonstrated on PC12 cells. Biotinylated fiber could be fabricated by biotinylating alginate before drawing fiber with WSC, enabling biotinylated NGF to be immobilized to fiber via an avidin bridge. The immobilized NGF induced the differentiation of PC12 cells seeded on the fiber. Bovine pulmonary endothelial cells, human dermal fibroblasts, and human mesenchymal stem cells were encapsulated, demonstrating good viability as determined by Live/Dead and WST-1 assays. The assembly of biostructural units into constructs was illustrated by using human mesenchymal stem cell-encapsulated fiber units. Cells in the resulting constructs could be induced to differentiate along chondrogenic and osteogenic lineages.

Alginates↗
PubMed2006

Self-assembled copper-capillary alginate gel scaffolds with oligochitosan support embryonic stem cell growth.

Biomaterial scaffolds are fundamental components of strategies aimed at engineering a wide range of tissues. Scaffolds possessing uniform, oriented microtubular architectures could be ideal for multiple tissues, but are challenging to produce. Therefore, we developed hydrogel scaffolds possessing regular, tubular microstructures from self-assembled copper-capillary alginate gel (CCAG). To abrogate the rapid dissolution of CCAG in cell culture media, we treated it with oligochitosan and created a stable oligochitosan-CCAG (OCCAG) polyelectrolyte complex. Fourier transform infrared spectroscopy confirmed polyelectrolyte complexation between alginate and oligochitosan. OCCAG retained capillary morphology, shrank anisotropically in bulk, lost Cu(2+) ions, and maintained (71.9 +/- 5.65)% of its mass in cell culture media. Next, we seeded mouse embryonic stem (ES) cells within OCCAG scaffolds, and examined cell morphology and quantified cell growth and viability over four days. ES cells were guided to form cylindrical structures of staggered cells within scaffold capillaries. Analysis of the total cells recovered from the scaffolds revealed exponential cell growth (normalized to day 0) that was statistically similar to gelatinized-plate controls. OCCAG-cultured ES cell viability was also not significantly different from controls at day 4. CCAG-derived scaffolds can therefore serve as a unique platform for stem cell-based tissue engineering.

Alginates↗
PubMed2006

Defoliation and plasmid delivery with layer-by-layer coated colloids.

The uptake of polyelectrolyte multilayer coated colloids into cells, subsequent defoliation and plasmid delivery was studied by means of confocal microscopy and flow cytometry. Silica particles coated layer-wise with protamine and dextran sulfate were given to HEK 293T cells. Optimum uptake was found with protamine as the top layer. The particle uptake likely follows an non-receptor-mediated endocytotic pathway. Defoliation of polyelectrolyte multilayer coated particles within cells was demonstrated by the release of incorporated plasmids as indicated by the expression of plasmid encoded proteins using the enhanced green fluorescence proteine (pEGFP-C1) plasmid and a red fluorescence protein (pDsRed1-N1) plasmid. This proves, together with the direct observation of fluorescent layer debris, the defoliation of coated particles and the release of layer components into the cytoplasm. Particle uptake and GFP expression.

Animals↗
PubMed2006

Bioengineering Functional Copolymers. IX. Poly[(maleic anhydride-co-hexene-1)-g-poly(ethylene oxide)].

Amphiphilic bioengineering copolymers having a combination of hydrophilic/hydrophobic linkages and polyelectrolyte behavior, along with an ability to interact with biomacromolecules, in particular with the invertase enzyme, have been synthesized by (a) complex-radical copolymerization of maleic anhydride (MA, the acceptor) and hexene-1 (H-1, the donor) monomers with benzoyl peroxide as the initiator in 1,4-dioxane at 65 degrees C under high-conversion conditions and (b) subsequent grafting (polyesterification) of synthesized poly(MA-alt-H-1) with alpha-methoxy-omega-hydroxy-poly(ethylene oxide) (PEO). Copolymerizations were also carried out in the steady state, in order to essentially reduce the effect of copolymer composition drift. The values of the monomer reactivity ratios (r(1) and r(2)) determined by using the known terminal models of Fineman-Ross (FR) and Kelen-Tüdös (KT), as well as by nonlinear regression (NLR) analysis, are: r(1) = 0.16 and r(2) = 0.30 (FR), r(1) = 0.14 and r(2) = 0.27 (KT), and r(1) = 0.15 and r(2) = 0.29 (NLR), respectively. All the copolymers and graft copolymers were characterized by FTIR spectroscopy, (1)H{(13)C} NMR spectroscopy, viscometric measurements, and chemical (acid number), thermal (DSC and TGA), and X-ray diffraction analyses. Unlike poly(MA-alt-H-1)s, PEO macrobranched graft copolymers exhibit expressed polyelectrolyte and swelling behavior in diluted and concentrated dioxane solutions, respectively. The copolymer and its PEO hyperbranched derivatives can be used as carriers for enzyme immobilization.

Enzymes, Immobilized↗
PubMed1992

The longitudinal relaxation time (T1) of the intracellular 23Na NMR signal in the isolated perfused rat heart during hypoxia and reoxygenation.

Each of six perfused rat hearts was subjected to 30 min of hypoxia followed by 60 min of reoxygenation. Inversion-recovery data on the intracellular Na NMR signal, differentiated by a shift reagent, 6 mM Dy(PPP)2, were obtained every 5 min, and T1 values were calculated. The T1 of the intracellular Na signal did not show any significant change either during hypoxia or upon reoxygenation, although the level of Nai increased about 50%. Such an increase of total Nai is expected to reduce the observed relaxation rate by diluting the fraction of Nai ions that interact with intracellular polyelectrolytes. The observed constancy of T1 in our study is explained on the basis of the typical values of the dissociation constants of sodium ions, in aqueous solutions, in interaction with polyelectrolytes. Although the constancy of intracellular sodium T1 during hypoxia may preclude the utilization of T1 weighting for the monitoring of pathology, its determination could be important for setting optimal acquisition times in high time-resolution experiments.

Animals↗
PubMed2002

Phosphates, DNA, and the search for nonterrean life: a second generation model for genetic molecules.

Phosphate groups are found and used widely in biological chemistry. We have asked whether phosphate groups are likely to be important to the functioning of genetic molecules, including DNA and RNA. From observations made on synthetic analogs of DNA and RNA where the phosphates are replaced by nonanionic linking groups, we infer a set of rules that highlight the importance of the phosphodiester backbone for the proper functioning of DNA as a genetic molecule. The polyanionic backbone appears to give DNA the capability of replication following simple rules, and evolving. The polyanionic nature of the backbone appears to be critical to prevent the single strands from folding, permitting them to act as templates, guiding the interaction between two strands to form a duplex in a way that permits simple rules to guide the molecular recognition event, and buffering the sensitivity of its physicochemical properties to changes in sequence. We argue that the feature of a polyelectrolyte (polyanion or polycation) may be required for a "self-sustaining chemical system capable of Darwinian evolution." The polyelectrolyte structure therefore may be a universal signature of life, regardless of its genesis, and unique to living forms as well.

DNA↗
PubMed1997

Electrostatic Interactions and Stability of Poly-l -lysine Covered Polystyrene Latex Particles Investigated by Dynamic Light Scattering

Adsorption isotherms of the pH dependent positively charged polyelectrolyte poly-l -lysine (PLL) on negatively and positively charged polystyrene latices are determined. With photon correlation spectrometry (PCS) the influence of the fluctuating PLL domaines in solution on the diffusion coefficient is observed at low salt concentrations c NaBr < 10(-3) M with lambda = c PE /c NaBr < 0.1 (c PE = concentration of the polyelectrolyte units). Screening of the charged layer by increasing electrolyte concentration results in large adsorbed amounts and layer thicknesses. At low molar mass of PLL the suspensions become unstable and the state and kinetic of flocculation is followed by the decreasing diffusion coefficient. PLL of higher molar mass (M w >/= 100 000) stabilizes the particles sterically and the adsorbed layer thicknesses can be determined. The conclusions drawn from PCS features are confirmed directly by raster electron micrographs of the filtered particles.

Journal Article↗
PubMed1998

Binding of Polycarboxylic Acids to Cationic Mixed Micelles: Effects of Polymer Counterion Binding and Polyion Charge Distribution.

Mixed micelles of cetyltrimethylammonium chloride (CTAC) and n-dodecyl hexaoxyethylene glycol monoether (C12E8) bind to polyanions when the mole fraction of the cationic surfactant exceeds a critical value (Yc). Yc corresponds to a critical micelle surface charge density at which polyelectrolyte will bind to this colloidal particle. Turbidimetric titrations were used to determine Yc for such cationic-nonionic micelles in the presence of acrylic acid and acrylamido-2-methylpropane sulfonate homopolymers (PAA and PAMPS, respectively) and their copolymers with acrylamide, as function of pH, ionic strength, and polyelectrolyte counterion. In 0.20 M NaCl, Yc for PAA is found to be remarkably insensitive to pH, i.e., virtually independent of the apparent polymer charge density xiapp. On the other hand, the expected inverse relationship between Yc and xiapp is observed either for PAA when NaCl is replaced by TMACl (tetramethylammonium chloride), or when xiapp is manipulated using acrylic acid/acrylamide copolymers at high pH. The effective charge density of PAA is thus seen to be suppressed by specific sodium ion binding, indicating that the influence of salts on the interaction of polycarboxylic acids with colloidal particles may differ qualitatively from their effect on the analogous behavior of strong polyanions. Comparisons between homo- and copolymers of acrylic acid were carried out also to test the hypothesis that the "mobility" of charges on PAA at moderate pH (degree of ionization less than unity) could make this "annealed" polymer exhibit the behavior of a more highly charged one. The results, while consistent with this expectation, were obscured by the likely effect of copolymer sequence distributions. Copyright 1998 Academic Press.

Journal Article↗
PubMed1999

Flocculation Studied with the ESA Technique.

The aim of this paper is to show that the ESA (electrokinetic sonic amplitude) technique can be used to study the flocculation between cationic polyelectrolytes and negatively charged silica particles. The ESA signal was measured when cationic polyacrylamide (CPAM) or cationic polyamine (POL) was mixed with silica particles. The dynamic mobility of the formed flocs was calculated from the corrected ESA signal. The amount of nonadsorbed polyelectrolyte was determined by viscosity. The floc sediment volume was also measured. It was found that the polyacrylamide molecule was more efficient than the polyamine molecule in neutralizing the charges on the silica particles due to the longer CPAM molecules and the larger distance between the CPAM charges which was in better accordance with the distance between the silica charges compared to POL. Copyright 1999 Academic Press.

Journal Article↗
PubMed1999

The Lower Cation Exchange Capacity Limit of Montmorillonite.

Wyoming montmorillonite (Volclay) with different charges were produced by Li-incorporation and the interlayer cations were replaced by tetramethyl ammonium. Their XRD pattern showed a regular sequence of expanded and collapsed interlayers. The regularly interstratified structure corresponds to a regularity of Reichweite R = 1. The expanded part of the interlayers was calculated by comparing XRD pattern with simulations using NEWMOD software. The calculations of the cation exchange capacity CEC for the expanded interlayer part gives a constant value of 65 +/- 2 mmol/100 g fully swellable montmorillonite. This value is denoted as the lower CEC limit of montmorillonite. We propose a model which considers montmorillonite to be a stacked two-dimensional polyelectrolyte. The model propose that interlayers of the stack collapse spontaneously by cation shifting into the neighboring interlayers, if the charge density of a montmorillonite has a value below the lower CEC value. The shifted cations of the collapsed interlayer increase the charge density in the neighboring interlayers and prevent their collapse. A regularly interstratified structure arises with the sequence expanded/collapsed/expanded interlayer, which can be observed by XRD. The behavior of low charged montmorillonite is explained with the properties of a two-dimensional polyelectrolyte. Below the critical layer charge, the Van der Waals forces dominate over electrostatic repulsive forces and the interlayers collapse. Copyright 1999 Academic Press.

Journal Article↗
PubMed1999

Electric Properties of Adsorbed Polystyrenesulfonate.

The influence of molecular weight on the counterion polarization of sodium polystyrenesulfonate (NaPSS) is investigated by electric light scattering. The polyelectrolyte is adsorbed in excess on beta-ferric hydrous oxide particles (beta-FeOOH), which are shown to assume the charge characteristics of the polymer. Two dispersion regions of the electro-optical effect (below and above 10 kHz) are found to exist due to the polarization of counterions. The high-frequency (HF) effect is attributed to polarization of free counterions along the polymer-coated particle axis and does not depend on the molecular weight of the adsorbed polymer. The amplitude and critical frequency of relaxation of the low-frequency (LF) effect, which is attributed to polarization of bound counterions along the polymer axis, depend on the polyelectrolyte molecular weight. The polarization of bound counterions seems to be responsible for the permanent-like dipole moment behavior of NaPSS at low frequencies of the applied electric field. Copyright 1999 Academic Press.

Journal Article↗
PubMed2000

Dielectric Relaxation Around a Charged Colloidal Cylinder in an Electrolyte.

The polarizability and corresponding dielectric relaxation of the Debye-Hückel (DH) atmosphere surrounding a charged rod-like polyelectrolyte immersed in an ionic solution of a symmetrical electrolyte is determined following the method developed by J. A. Fornés [Phys. Rev. E 57, 2110 (1998)]. Several formulas are given to estimate the DH atmosphere parameters, namely, the polarizability at zero frequency, alpha(0), the relaxation time, tau, the cloud capacitance, C, the average displacement of the ionic cloud, delta, the square root dipole moment quadratic fluctuation, (1/2), and the thermal fluctuating field, (1/2). The Poisson-Boltzmann equation is solved numerically to apply the theory to a highly charged polyelectrolyte such as DNA in solution, although formulas valid for the DH approximation are also given. A dispersion in the polarizability and correspondingly in the dielectric constant of these solutions in the microwave region is predicted. For instance, considering a DNA length of 1000 Å, with its reduced linear charge density xi(0)=4.25 and ionization factor gamma=0.5, immersed in a NaCl solution (40 mM), we predict a polarizability of the DH atmosphere at zero frequency alpha(0) of 1x10(-33) Fm(2) ( approximately 6.1x10(6)) times greater than the mean value of the polarizability of water) and the corresponding fluctuating dipole moment p of 2.1x10(-27) Cm ( approximately 600 times greater than the permanent dipole moment of water molecule). The relaxation time and the average displacement of the ionic cloud are tau=1.6 ns and delta=14. Å, respectively. This displacement is produced by the thermal fluctuating field, which, in this case, at room temperature is (1/2)=2 x10(6) V/m. Copyright 2000 Academic Press.

Journal Article↗
PubMed2000

Electrophoretic Mobility of Soft Particles in Concentrated Suspensions.

A general theory is developed for the electrophoretic mobility of spherical soft particles (i.e., spherical hard colloidal particles of radius a coated with a layer of polyelectrolytes of thickness d) in concentrated suspensions in an electrolyte solution as a function of the particle volume fraction &phi; on the basis of Kuwabara's cell model. In the limit d-->0, the mobility expression obtained tends to that for spherical hard particles in concentrated suspensions, whereas in the limit a-->0, it becomes that for spherical polyelectrolytes (charged porous spheres with no particle core). Simple approximate analytic mobility expressions are derived for the case where relaxation effect is negligible. It is found that in practical cases, the &phi; dependence of the mobility is negligible for d< >a, the mobility strongly decreases with increasing &phi;. Copyright 2000 Academic Press.

Journal Article↗
PubMed2000

Electrical Conductivity of a Concentrated Suspension of Soft Particles.

A general expression for the electrical conductivity of a concentrated suspension of spherical soft particles (polyelectrolyte-coated particles) is obtained for the case where the overlapping of the electrical double layers of adjacent particles is negligible by using Kuwabara's cell model. It is shown that in the limit of very low potentials the obtained conductivity expression reduces to Maxwell's relation with respect to the volume fraction of the particle core and the contribution from the polyelectrolyte layer becomes negligible. An approximate conductivity expression is derived for the case of low potentials. Copyright 2000 Academic Press.

Journal Article↗
PubMed2000

Normal Forces between Cellulose Surfaces Measured with Colloidal Probe Microscopy.

Colloidal probe microscopy was employed to study interactions between cellulose surfaces in aqueous solutions. Hydrodynamic forces must be accounted for in data analysis. Long-range interactions betweeen cellulose surfaces are governed by double-layer forces and, once surfaces contact, by osmotic repulsive forces and viscoelasticity. Increasing the ionic strength decreases surface potentials and increases adhesive forces. Polyelectrolytes cause strong steric repulsion at high surface coverage, where interactions are sensitive to probe velocity. Polymer bridging occurs at low coverage. The conformation of adsorbed polyelectrolytes depends on the polymer concentration. Copyright 2000 Academic Press.

Journal Article↗
PubMed1985

Toward molecular electronics. Self-screening of molecular wires.

One-dimensional polyelectrolytes are proposed as molecular devices based on soliton propagation. The use of such "molecular wires" as delay lines or shift registers raises the problem of their electrical screening, because, when a large number of these wires are densely packed, cross-talking between them might occur. In order to overcome such a drawback, a detailed study of the polyelectrolyte behavior in an ionic solution has been developed, under equilibrium conditions. The results bring into evidence a condensation process, around each molecular wire, of the mobile ions in the solution. The consequent self-screening effect could be relevant in reducing cross-talking.

Chemical Phenomena↗