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At least 793 records · Page 44Linked to original sources
PubMed2006

Interaction between the conjugated polyelectrolyte poly{1,4-phenylene[9,9-bis(4-phenoxybutylsulfonate)]fluorene-2,7-diyl} copolymer and the lecithin mimic 1-O-(l-Arginyl)-2,3-O-dilauroyl-sn-glycerol in aqueous solution.

In this paper, the interaction between the water-soluble conjugated polyelectrolyte poly{1,4-phenylene[9,9-bis(4-phenoxybutylsulfonate)]fluorene-2,7-diyl} copolymer and the amino acid glyceride conjugate 1-O-(L-arginyl)-2,3-O-dilauroyl-sn-glycerol dichlorohydrate (a mimic for the phospholipid lecithin) has been studied in aqueous solution by electronic spectroscopy (absorption and fluorescence) and small-angle neutron scattering (SANS). A significant increase in the polymer fluorescence and blue shift in its emission are observed on association with the surfactant. This is suggested to be due to breakup of polymer aggregates. In addition, the spectroscopic and photophysical data suggest this is followed by the vesicle to ribbon transition characteristic of this surfactant, leading to incorporation of single chains of the polymer within mixed polymer-surfactant aggregates. Support for this comes from preliminary SANS measurements, from which evidence for polymer dissolution and formation of two-dimensional structures has been obtained.

Journal Article↗
PubMed2006

Mineralization of monodispersed CdS nanoparticles on polyelectrolyte superstructure forming an electroluminescent "necklace-of-beads".

We report a nonmicellar method to synthesize monodisperse semiconducting nanoparticles templated on polymer chains dissolved in solution at high yield. The monodispersity is achieved due to the beaded necklace morphology of the polyelectrolyte chains in solution where the beads are nanometer-scale nodules in the polymer chain. The resultant structure is a nanoparticles studded necklace where the particles are imbedded in the beads. Multiple cycles of synthesis on the polymer template yield nanoparticles of identical size, resulting in a nanocomposite with high particle fraction. The resultant nanocomposite has beaded-fibrilar morphology with imbedded nanoparticles and can be solution-casted to make electroluminescent thin film device.

Cadmium Compounds↗
PubMed2007

Nanostructure and transition of a strong polyelectrolyte brush at the air/water interface.

The strong polyelectrolyte layer in the monolayer of ionic amphiphilic diblock copolymers at the air/water interface consists of carpet and brush layers when the brush density is satisfactorily high like that of the weak acid polymer. Also, a drastic structural change was induced by the addition of salt to the brush layer. In this study, the critical brush density for the transition between "carpet-only" and "carpet + brush" structures for the strongly ionic amphiphilic diblock copolymer, poly(hydrogenated isoprepene)-b-poly(styrene sulfonic acid) sodium salt, monolayer was measured by an in situ X-ray reflectivity technique. The critical brush density was found to be about 0.12 nm-2, which is lower than that observed for a weak acid polymer and, unlike the weak acid polymer, is independent of the hydrophilic chain length. This difference might be attributed to the strong ionic nature of the brush chain. In addition, the reversibility of the transition was confirmed. The effect of salt addition to the nanostructure of the carpet layer was examined in detail. No structural change was found, indicating that most of the ionic groups in the carpet layer do not show an ionic nature because of counterion condensation.

Anions↗
PubMed2007

Layer-by-layer assembly of pH-responsive, compositionally controlled (co)polyelectrolytes synthesized via RAFT.

Homo- and block copolyelectrolytes that have well-defined structures and are responsive to pH were synthesized via reversible addition-fragmentation chain-transfer (RAFT) polymerization and employed to produce layer-by-layer (LBL) films. Acrylamido monomers with carboxylate, sulfonate, and amine functionality were utilized to provide both strong and weak homopolyelectrolytes and mixed strong/weak copolyelectrolyte systems. Multilayer films were prepared under specified conditions of pH and ionic strength and analyzed via atomic force microscopy and ellipsometry to study the effects of changes in the local molecular environment on film morphologies. The pH responsiveness and integrity of the multilayer assemblies were investigated by exposing films to solutions of varying pH in a fluid cell and performing in situ AFM analysis. The multilayer dimensions, morphology, and integrity were found to depend on the molecular architecture of the polyelectrolytes, with changes in segmental type and repeating unit distribution producing dramatic differences in film characteristics. These results suggest the possibility of producing LBL assemblies of precisely controlled dimensions and properties by specifically tailoring copolymer structure. To our knowledge, this is the first report of LBL assembly of RAFT-synthesized homo- and copolyelectrolyte multilayer complexes.

Journal Article↗
PubMed2007

Counterions and water in polyelectrolyte multilayers: a tale of two polycations.

Attenuated total internal reflectance Fourier transform infrared, ATR-FTIR, spectroscopy was used to compare the water uptake and doping within polyelectrolyte multilayers made from poly(styrene sulfonate), PSS, and a polycation, either poly(allylamine hydrochloride), PAH, or poly(diallyldimethylammonium chloride), PDADMAC. Unlike PDADMA/PSS multilayers, whose water content depended on the solution ionic strength, PAH/PSS multilayers were resistant to doping by NaCl to a concentration of 1.2 M. Using (infrared active) perchlorate salt, the fraction of residual counterions in PDADMA/PSS and PAH/PSS was determined to be 3% and 6%, respectively. The free energy of association between the polymer segments, in the presence of NaClO4, was about 5 kJ mol-1 and -10 kJ mol-1, respectively, for PDADMA/PSS and PAH/PSS, indicating the relatively strong association between the polymer segments in the latter relative to the former. Varying the pH of the solution in contact with the PAH/PSS multilayer revealed a transition to a highly swollen state, interpreted to signal protonation of PAH under much more basic conditions than the pKa of the solution polymer. The increase in the multilayer pKa suggested an interaction energy for PAH/PSS in NaCl of ca. 16 kJ mol-1.

Journal Article↗
PubMed2006

Decomposing bridging adhesion between polyelectrolyte layers into single molecule contributions.

A novel approach to analyze the force response of multiple polymer strands, which are bridged between two surfaces, is proposed. The response of single polymer strands is experimentally accessible by measuring the force upon separation of two polymer-coated surfaces with the atomic force microscope. Our approach is based on the decomposition of the stretching and desorption sequence into contributions of independently bridged chains and of the elimination of loops formed on the opposite surface during contact. This approach was applied to investigate the bridging adhesion of surfaces coated with poly(vinylamine) (PVA). The force response of single PVA molecules was described on the basis of a recently proposed model, which accounts for the discrete chain character of the polymer at higher extension forces. As exemplary results, we determined the length distributions of the individual chains and the loop number distribution of these bridging chains on the polyelectrolyte-coated surfaces. The former were compared with scaling theories of polymer adsorption.

Journal Article↗
PubMed2005

Chemically nanopatterned surfaces using polyelectrolytes and ultraviolet-cured hard molds.

Polymer transfer printing of poly(acrylic acid) onto a polyelectrolyte multilayer platform resulted in chemically nanopatterned surfaces with well-defined structures and both positive and negative surface functionalities. A commercially available urethane-related photopolymer cured by ultraviolet light was used to make stamps for contact printing with a range of submicrometer down to 80 nm features because of its outstanding mechanical stability and inherent softening transition above 48 degrees C.

Acrylic Resins↗
PubMed2005

DNA multilayer films on planar and colloidal supports: sequential assembly of like-charged polyelectrolytes.

Multilayer films comprising solely negatively charged polyelectrolytes were sequentially assembled based on DNA hybridization. Films prepared from alternating layers of two-block homopolymeric nucleotides (polyA(20)G(20)/polyT(20)C(20)) grew linearly with increasing layer number, as verified by quartz crystal microgravimetry, UV-vis spectrophotometry and optical microscopy. Urea treatment of the films induced morphological changes, while exposure to low ionic strength solutions resulted in film disassembly. DNA multilayer films were also formed on silica particles, and DNA hollow capsules were obtained following dissolution of the template core.

Adsorption↗
PubMed2005

Single molecular imaging and spectroscopy of conjugated polyelectrolytes decorated on stretched aligned DNA.

DNA is the prototype template for building nanoelectronic devices by self-assembly. The electronic functions are made possible by coordinating electronic polymer chains to DNA. This paper demonstrates two methods for fabrication of aligned and ordered DNA nanowires complexed with conjugated polyelectrolytes (CPEs). The complex can be formed either in solution prior to stretching or after stretching of the bare DNA on a surface. Molecular combing was used to stretch the complexes on surface energy patterned surfaces, and PMMA for the bare DNA. Single molecular spectroscopy, in fluorescence, and microscopy, in atomic force microscopy, give evidence for coordination of the short CPE chains to the aligned DNA.

DNA↗
PubMed2006

Distance-dependent fluorescence quenching on gold nanoparticles ensheathed with layer-by-layer assembled polyelectrolytes.

We report on the preparation, characterization, and photophysical study of new fluorescent core/shell nanoparticles fabricated by electrostatic layer-by-layer assembly. On the basis of gold cores with a diameter of 13 nm, these nanocolloids possess different fluorescently labeled polymer corona layers at various distances from the surface of the core metal using nonfluorescent polyelectrolytes as spacer layers. UV-visible spectroscopy and transmission electron microscopy confirm that the particle suspensions of fluorescently labeled core/shell nanoparticles are stable at all stages of their construction. Photophysical investigations reveal strongly distance-dependent fluorescence quenching in these particle systems. The contribution of the metal core to this quenching can be assesed precisely after the gentle dissolution of the gold cores by potassium cyanide. The photophysical measurements reveal clearly that the gold nanoparticles decrease the transition probability for radiative transitions.

Journal Article↗
PubMed2006

Cationic dithieno[3,2-b:2',3'-d]phospholes: a new building block for luminescent, conjugated polyelectrolytes.

Cationic dithieno[3,2-b:2',3'-d]phospholes are accessible very efficiently by methylation of the phosphorus center. Further functionalization with bromo substituents in 2,6-positions affords a polymerizable monomer that can be copolymerized with a difunctionalized fluorene in a Suzuki-Miyaura-type cross-coupling protocol. The monomers as well as the resulting conjugated polyelectrolyte based on the phospholium units show very intriguing photoluminescence properties, even in the solid state. [structure: see text]

Journal Article↗
PubMedDate not supplied

Affinity precipitation of monoclonal antibodies by nonstoichiometric polyelectrolyte complexes.

The nonstoichiometric polyelectrolyte complex (PEC) formed by poly(methacrylic acid) (degree of polymerization 1830) (PMAA) and poly(N-ethyl-4-vinyl-pyridinium bromide) (degree of polymerization 530) (PEVP) undergoes reversible precipitation from aqueous solution at any desired pH-value in the range 4.5-6.5 depending on the ionic strength and PEVP/PMAA ratio in the complex. The antigen, inactivated glyceraldehyde-3-phosphate dehydrogenase (GAPDH) from rabbit was covalently coupled to PEVP. The resulting GAPDH-PEVP/PMAA complex was used for the purification of antibodies from a 6G7 clone specific towards inactivated GAPDH. The crude extract was incubated with GAPDH-containing PEC and the precipitation of the PEC was carried out at 0.01 M NaCl and pH 4.5, 5.3, 6.0 and 6.5 using PEC with PEVP/PMAA ratios of 0.45, 0.3, 0.2 and 0.15, respectively. Purified antibodies were eluted at pH 4.0 where PECs of all compositions used were insoluble. PEC precipitation is accompanied only by small nonspecific coprecipitation of proteins. Precipitated PEC could be dissolved at pH 7.3 and used repeatedly.

Animals↗
PubMed1998

Studies on the setting of polyelectrolyte cements: part VI. The effect of halide salts on the mechanical properties and water balance of zinc polycarboxylate and glass-ionomer dental cements.

A study is reported in which a zinc polycarboxylate and a glass polyalkenoate dental cement, respectively, were prepared from aqueous solutions of NaCl, KCl, KBr and KI, all at 1 mol dm3 concentration, as well as from pure water. For the zinc polycarboxylate, setting as determined by oscillating rheometry was speeded up and water uptake was enhanced by the presence of the salts. Conversely, compressive strength at 24 h was unaffected. On the other hand, for the glass polyalkenoate, the setting reaction was slowed down, water uptake inhibited and compressive strength at 24 h reduced (from 94.3 MPa with pure water to 59.8 MPa with NaCl, 65.8 MPa for KCl, 67.0 MPa for KBr and 81.1 MPa for KI). Previous work with polyelectrolytes in aqueous solution suggests that the halides probably enhance the rate of the neutralization process. For the zinc polycarboxylate, this leads to a more rapid setting reaction. By contrast, for the glass polyalkenoate, it results in slower setting and weaker cements. This result is attributed to inhibition of the secondary setting reaction, involving the formation of the silicate/phosphate network, by enhanced neutralization, a process which is consequently concluded to occur earlier in the overall setting of these cements than had been assumed previously.

Journal Article↗
PubMed1996

The effect of hydrophobic character of drugs and helix-coil transition of kappa-carrageenan on the polyelectrolyte-drug interaction.

PURPOSE: The extent of adsorption of different drug molecules to kappa-carrageenan was investigated in order to evaluate the effect of drug hydrophobicity on the adsorption isotherm. METHOD: Dialysis experiments were used to determine the amount of drug adsorbed to the polyelectrolyte. The amount of drug on both sides of the membrane was determined spectrophotometrically after attaining equilibrium. CMC for the drugs were determined by the dye solubilisation method. RESULTS: It is shown that the small differences in structure between the drug molecules used in this study still leads to considerable difference in adsorption properties, especially the onset of adsorption. It was also found that the slope of the adsorption isotherms among the drug molecules followed the same pattern as the CMC values for drugs. The extent of adsorption of drugs to the helix from of kappa-carrageenan was much higher than to the coil form. CONCLUSIONS: These results suggest that the adsorption of charged drug molecules to an oppositely charged polymer is effected not only by the coulombic interactions, but also by the hydrophobicity of the drug. Furthermore, the adsorption of drug molecules to kappa-carrageenan in the helix form is higher than for the coil form because of the shorter distance between the charges and the thereby enhanced hydrophobic interaction between bound drug molecules.

Adsorption↗
PubMed2004

Encapsulation of catalase in polyelectrolyte microspheres composed of melamine formaldehyde, dextran sulfate, and protamine.

Immobilization of catalase (molecular weight 240,000 daltons) in polyelectrolyte microspheres was studied. The microspheres were obtained by alternating adsorption of dextran sulfate and protamine on commercially available melamine formaldehyde cores followed by the core hydrolysis at pH 1.7. As the interior of the microspheres was filled with homogeneous matrix, the catalase distribution inside the microspheres was uniform. The quantity of entrapped catalase was dependent on the initial concentration of the enzyme and pH of solution, and the peak value was 10(8)-10(9) molecules per microsphere. It was demonstrated that catalase was entrapped in the microspheres via electrostatic and hydrophobic interactions. The catalase activity inside the microspheres increased as the quantity of enzyme decreased, which was due to the switch between diffusion and kinetic regimes of the enzymatic reaction. The microspheres could be applied for separation and concentration of high molecular weight proteins.

Catalase↗
PubMed1978

Apparent antihaemophilic activity of basic amphoteric polyelectrolytes.

Amphoteric polyelectrolytes with alkaline isoelectric points (for example Ampholine 9-11) intended for use in isoelectric focussing were found to shorten the prolonged partial thrombosplastin clotting time with kaolin (PTTK) of plasma deficient in factor VIII. The response of this PTTK to Ampholine 9-11 was linear when plotted on double log paper with a slope slightly greater than that of factor VIII itself. Ampholine 9-11 at 2% concentration had factor VIII and factor IX activity equal to that of normal plasma as well as somewhat less activity as factor XI. It had no significant correcting effect on the clotting of plasmas deficient in factors V, VII, X, II OR XII. Ampholine 9-11 inhibited low concentrations of contact activators and its effect in correcting factor VIII deficient plasma was found to be related to the degree of contact activation.

Amino Acids↗
PubMed2003

The zwitterion effect in high-conductivity polyelectrolyte materials.

The future of lithium metal batteries as a widespread, safe and reliable form of high-energy-density rechargeable battery depends on a significant advancement in the electrolyte material used in these devices. Molecular solvent-based electrolytes have been superceded by polymer electrolytes in some prototype devices, primarily in a drive to overcome leakage and flammability problems, but these often exhibit low ionic conductivity and prohibitively poor lithium-ion transport. To overcome this, it is necessary to encourage dissociation of the lithium ion from the anionic polymer backbone, ideally without the introduction of competing, mobile ionic species. Here we demonstrate the effect of zwitterionic compounds, where the cationic and anionic charges are immobilized on the same molecule, as extremely effective lithium ion 'dissociation enhancers'. The zwitterion produces electrolyte materials with conductivities up to seven times larger than the pure polyelectrolyte gels, a phenomenon that appears to be common to a number of different copolymer and solvent systems.

Complex Mixtures↗
PubMed2002

Reversibly erasable nanoporous anti-reflection coatings from polyelectrolyte multilayers.

For nearly two centuries, researchers have sought novel methods to increase light transmission in optical systems, as well as to eliminate unwanted reflections and glare. Anti-reflection coatings and surfaces have enabled the increasing performance demands of optical components fabricated from glass-based optical materials. With the current trend of technology moving towards optically transparent polymeric media and coatings, the need for anti-reflection technology and environmentally benign processing methods for polymeric materials independent of shape or size has become quite apparent. We describe an economical, aqueous-based process controlled at the molecular level that simultaneously coats all surfaces of almost any material. Systematically designed nanoporous polymer films are used, which are suitable for optical applications operating at both visible and near-infrared wavelengths. These high-efficiency anti-reflection coatings are created from phase-separated polyelectrolyte multilayer films that undergo a reversible pH-induced swelling transition. Furthermore, such films, easily patterned by an inkjet printing technique, possess potential for pH-responsive biomaterial and membrane applications.

Journal Article↗