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PubMed2006

Spectroscopic investigation of the adsorption mechanisms of polyacrylamide polymers onto iron oxide particles.

The mechanisms of high-molecular-weight polyacrylamide nonionic homopolymer and 25 mol% anionic acrylate-substituted copolymer adsorption onto iron oxide particles were investigated via DRIFT and UV-vis spectroscopies at three pH values (6, 8.5, and 11). While electrostatic interactions play an important role in charged polymer adsorption, this information is not spectroscopically available. At pH values above and below pH 8.5 (the isoelectric point for the anionic polymer), bidentate chelation and hydrogen bonding were the main adsorption mechanisms. At the isoelectric point, monodentate chelation was observed to be the main mode of adsorption, along with hydrogen bonding. For the nonionic polymer, in all cases, hydrogen bonding through the carbonyl group was the main mode of adsorption. The adsorption of both polymers conformed well to the Freundlich model, suggesting that the adsorbed polymer amount increases with increasing polymer concentration up to 7500 g/t solid, rather than approaching monolayer coverage. Spectroscopic evidence was found to suggest that hydrolysis of nonionic polyacrylamide occurs at high pH.

Journal Article↗

PubMed2006

Estimation of polymer-surface interfacial interaction strength by a contact AFM technique.

Atomic force microscopy (AFM) measurements were employed to assess polymer-surface interfacial interaction strength. The main feature of the measurement is the use of contact-mode AFM as a tool to scratch off the polymer monolayer adsorbed on the solid surface. Tapping-mode AFM was used to determine the depth of the scraped recess. Independent determination of the layer thickness obtained from optical phase interference microscopy (OPIM) confirmed the depth of the AFM scratch. The force required for the complete removal of the polymer layer with no apparent damage to the substrate surface was determined. Polypropylene (PP), low-density polyethylene (PE), and PP-grafted-maleic anhydride (PP-g-ma) were scraped off silane-treated glass slabs, and the strength of surface interaction of the polymer layer was determined. In all cases it was determined that the magnitude of surface interaction force is of the order of van der Waals (VDW) interactions. The interaction strength is influenced either by polymer ability to wet the surface (hydrophobic or hydrophilic interactions) or by hydrogen bonding between the polymer and the surface treatment.

Adsorption↗

PubMed2006

Dissolved organic nitrogen removal during water treatment by aluminum sulfate and cationic polymer coagulation.

Coagulation of three surface waters was conducted with aluminum salt and/or cationic polymer to assess dissolved organic nitrogen (DON) removal. Coagulation with aluminum sulfate removed equal or slightly lower amounts of DON as compared to dissolved organic carbon (DOC). At aluminum sulfate dosages up to 5mg per mg DOC, the cationic polymer improved DON removal by an additional 15% to 20% over aluminum sulfate alone. At very high aluminum sulfate dosages (>8 mg aluminum sulfate per mg DOC), however, the cationic polymer addition negligibly increased DON removal. Molecular weight fractionation before and after coagulation experiments indicated that cationic polymer addition can increase the removal of all molecular weight fractions of DON with the highest molecular weight fraction (>10,000 Da) being preferentially removed. Results indicated that the DON added as part of the cationic polymer was almost completely removed at optimum aluminum sulfate and polymer doses.

Alum Compounds↗

PubMed2002

Interaction of human serum albumin with membranes containing polymer-grafted lipids: spin-label ESR studies in the mushroom and brush regimes.

The adsorption of human serum albumin (HSA) to dipalmitoyl phosphatidylcholine (DPPC) bilayer membranes containing poly(ethylene glycol)-grafted dipalmitoyl phosphatidylethanolamine (PEG-DPPE) was studied as a function of content and headgroup size of the polymer lipid. In the absence of protein, conversion from the low-density mushroom regime to the high-density brush regime of polymer-lipid content is detected by the change in ESR outer hyperfine splitting, 2A(max), of chain spin-labelled phosphatidylcholine in gel-phase membranes. The values of 2A(max) remain constant in the mushroom regime, but decrease on entering the brush regime. Conversion between the two regimes occurs at mole fractions X(PEG)(m-->b) approximately 0.04, 0.01-0.02 and 0.005-0.01 for PEG-DPPE with mean PEG molecular masses of 350, 2000 and 5000 Da, respectively, as expected theoretically. Adsorption of HSA to DPPC membranes is detected as a decrease of the spin label 2A(max) hyperfine splitting in the gel phase. Saturation is obtained at a protein/lipid ratio of ca. 1:1 w/w. In the presence of polymer-grafted lipids, HSA adsorbs to DPPC membranes only in the mushroom regime, irrespective of polymer length. In the brush regime, the spin-label values of 2A(max) are unchanged in the presence of protein. Even in the mushroom regime, protein adsorption progressively becomes strongly attenuated as a result of the steric stabilization exerted by the polymer lipid. These results are in agreement with theoretical estimates of the lateral pressure exerted by the grafted polymer in the brush and mushroom regimes, respectively.

1,2-Dipalmitoylphosphatidylcholine↗

PubMed1996

High-efficiency loading, transfection, and fusion of cells by electroporation in two-phase polymer systems.

A method to concentrate drugs, DNA, or other materials with target cells in two-phase polymer systems for high-efficiency electroloading is described. The two-phase polymer system is utilized for cell and loading material selection, as well as for cell aggregation before electrofusion. The phase mixing of several water-soluble polymers is characterized, and the polyethylene glycol-Dextran (PEG m.w. 8,000 + Dextran m.w. 71,000) mixture is selected to illustrate the advantage of the two-phase systems. Fluorescently labeled Dextran or DNA is loaded into Chinese hamster ovary (CHO) and JTL cells, using electroporation in either the two-phase polymer system or the conventional single-phase suspension. The loading efficiency is 4 to 30 times higher for the two-phase system, with the best advantage at lower applied field range. Transfections of CHO, COS, Melan C, and JTL lymphoid cells using pSV-beta-galactosidase (for CHO and COS), pBK-RSV-tyrosinase, and pCP4-fucosidase plasmids, respectively, by electroporation in the two-phase polymer system and the conventional single-phase electroporation method, are compared. The former method is far superior to the latter in terms of efficiency. The threshold and optimal field strengths for the former are significantly lower than those for the latter method, so the former method is more favorable in terms of equipment requirement and safety. Electrofusion efficiency in the two-phase system is comparable to that in polyethylene glycol suspension alone and is a significant improvement from the conventional electrofusion method with dielectrophoresis. The two-phase polymer method is, therefore, a valuable technique for gene delivery to a limited cell source, as in ex vivo gene therapy.

Animals↗

PubMed1999

Sickle hemoglobin polymer melting in high concentration phosphate buffer.

Sickle cell hemoglobin (HbS) prepared in argon-saturated 1.8 M phosphate buffer was rapidly mixed with carbon monoxide (CO)-saturated buffer. The binding of CO to the sickle hemoglobin and the simultaneous melting of the hemoglobin polymers were monitored by transmission spectroscopy (optical absorption and turbidity). Changes in the absorption profile were interpreted as resulting from CO binding to deoxy-HbS while reduced scattering (turbidity) was attributed to melting (depolymerization) of the HbS polymer phase. Analysis of the data provides insight into the mechanism and kinetics of sickle hemoglobin polymer melting. Conversion of normal deoxygenated, adult hemoglobin (HbA) in high concentration phosphate buffer to the HbA-CO adduct was characterized by an average rate of 83 s-1. Under the same conditions, conversion of deoxy-HbS in the polymer phase to the HbS-CO adduct in the solution phase is characterized by an average rate of 5.8 s-1 via an intermediate species that grows in with a 36 s-1 rate. Spectral analysis of the intermediate species suggests that a significant amount of CO may bind to the polymer phase before the polymer melts.

Adult↗

PubMed2003

Viscosity function in polymer-modified asphalts.

Asphalt is a multidisperse micellar system with rheological behavior resembling that of a low-molecular-weight polymer. Nowadays, asphalt is frequently modified by blending it with various polymers. Such modified asphalt has rheological properties that differ from the properties of the base asphalt. It is quite common to study asphalt in dynamic experiments. Such studies, however useful, cannot reveal all characteristic features of polymer-modified asphalts. Asphalt modification by polymers is strongly manifested in the region of transitions from a viscoelastic fluid to the Newtonian fluid. The viscosity study in this region can reveal behavior characteristic of the used polymer modifier, thus complementing the dynamic studies of these materials. The viscosity of base asphalt modified by styrene-butadiene-styrene and by ethylene-vinyl acetate polymers (in several concentrations) is studied and discussed in this note.

Journal Article↗

PubMed2003

Polarizability and complex conductivity of dilute suspensions of spherical colloidal particles with uncharged (neutral) polymer coatings.

The polarizability of polymer-coated colloidal particles, as measured via dielectric relaxation spectroscopy, reflects on the degree to which convection, diffusion, and electromigration deform the equilibrium double layer. With a polymer coating, convection and electro-osmosis are resisted by hydrodynamic drag on the polymer segments. The electro-osmotic flow near the underlying bare surface is therefore diminished. Characteristics of the particles and the adsorbed polymer can, in principle, be inferred by measuring the frequency-dependent polarizability. In this work, "exact" numerical solutions of the electrokinetic equations are used to examine how adsorbed polymer changes the particle polarizability and, hence, the conductivity and dielectric constant increments of dilute suspensions. For neutral polymer coatings, the conductivity and dielectric constant increments are found to be very similar to those of the underlying bare particles, so the response depends mostly on the underlying bare particles. These observations suggest that dielectric spectroscopy is best used to determine the underlying surface charge, with characteristics of the coating inferred from the electrophoretic or dynamic mobility, together with the hydrodynamic radius obtained from sedimentation or dynamic light scattering. Addressed briefly are the effects of added counterions and nonspecific adsorption. The electrokinetic model explored in this work can be used to guide experiments (frequency and ionic strength, for example) to either minimize or maximize the sensitivity of the complex conductivity to the coating thickness or permeability.

Journal Article↗

PubMed2000

Oral peptide drug delivery: polymer-inhibitor conjugates protecting insulin from enzymatic degradation in vitro.

A drug-carrier matrix has been developed which protects embedded insulin from degradation by the luminally secreted serine-proteases trypsin (EC 3.4.21.4), chymotrypsin (EC 3.4.21.1) and elastase (EC 3.4.21.36) in vitro. Increasing amounts of the Bowman-Birk inhibitor (BBI) and elastatinal, respectively, were thereby covalently bound to the mucoadhesive polymer sodium carboxymethylcellulose (Na-CMC). The inhibitory efficacy of resulting polymers was evaluated. On the one hand, all polymer-BBI conjugates showed a strong inhibitory activity towards trypsin and chymotrypsin whereas it was markedly lower towards elastase. The polymer-elastatinal conjugates, on the other hand, displayed a comparatively higher inhibitory activity towards elastase. In an artificial intestinal fluid containing trypsin, chymotrypsin and elastase in physiological concentrations insulin, being incorporated in unmodified Na-CMC, was rapidly degraded at 37 degrees C. Within 1 h 98.7 +/- 0.4% (mean +/- SD, n = 3) of the peptide drug were thereby metabolized. On the contrary, the incorporation of insulin in a mixture of the two polymer-inhibitor conjugates CMC-BBI (40%; w/w) and CMC-elastatinal conjugate (60%; w/w) led to a peptide degradation of 22.3 +/- 2.5% (mean +/- SD, n = 3) within the same time period. Even after 4 h of incubation, 33.6 +/- 3.2% (mean +/- SD, n = 3) of the therapeutic agent remained stable towards enzymatic attack. Hence, the polymer-inhibitor conjugates described in this study seem to be a useful tool in overcoming the luminal enzymatic barrier in peroral insulin delivery.

Administration, Oral↗

PubMed2001

Water absorption and surface properties of novel poly(ethylmethacrylate) polymer systems for use in bone and cartilage repair.

The surface and bulk properties of novel methacrylate polymers prepared by gelling poly(ethyl methacrylate) (PEMA) powder with different ratios of tetrahydrofurfuryl methacrylate (THFMA) and hydroxyethyl methacrylate (HEMA) monomers were investigated. The water adsorption and desorption characteristics of these polymers were measured in water and phosphate buffered saline (PBS). The desorption diffusion coefficients were higher than the adsorption coefficients in both water and PBS. Linear relationships between the equilibrium mass of water taken up and the mass of water desorbed with the concentration of HEMA in the polymer were established. Polymer surfaces were analysed using scanning electron microscopy (SEM) and atomic force microscopy (AFM). Surface features varied with polymer composition; during hydration only selective areas of the surface hydrated indicating a heterogeneous surface. Contact angle data showed no trend between the different polymers indicating that contact angles are not an acceptable method of assessing hydrophobicity/wettability of a material which does not have a homogeneous surface. The effect of these bulk and surface characteristics on biological interactions were examined using bovine chondrocytes and human osteoblast (HOB) cell cultures. Cell attachment decreased when HEMA was present in the copolymer.

Absorption↗

PubMed1998

Effects of anionic and nonionic polymers on fusion and binding of Sendai virus to human erythrocyte ghosts.

Effects of various polymers (dextran sulfate, dextran and polyethylene glycol) on binding and fusion of Sendai virus to target cells were studied by use of fluorescence spectroscopy. Direct binding of dextran sulfate but not dextran to Sendai virus was detected. Anionic and nonionic polymers showed definite effects on segmental motions of the viral envelope proteins. Sendai virus binding to human erythrocyte ghost membranes (HEG) was reduced by dextran sulfate and dextran while the fusion temperature dependence remained unaltered at approximately 20 degrees C. Nonionic polymer, polyethylene glycol, caused an increase in extent of fusion of Sendai virus with HEG. Segmental motion of viral envelope proteins, determined in terms of anisotropy of fluorescent probes attached to viral surface proteins, exhibited a temperature dependent transition at 20 degrees C by a sharp change from restricted to less restricted motion. In the presence of each of the polymers, this transition was no longer apparent. Since fusion did occur in the presence of all polymers, the temperature dependent characteristic of Sendai virus target cell fusion can be said not to depend on viral surface protein segmental motion. A reasonable and coherent explanation was given for the apparent disparity between the effects of inhibiting and enhancing polymers on fusion and motion of viral proteins.

Animals↗

PubMed2000

An atomic force microscopy investigation of bioadhesive polymer adsorption onto human buccal cells.

Atomic force microscopy (AFM) was used to examine the buccal cell surface in order to image the presence of adsorbed bioadhesive polymers identified from previous work. Isotonic saline solution (5 ml) containing either polycarbophil (pH 7.6), chitosan (pH 4.5) or hydroxypropyl methylcellulose (pH 7.6) (0.5% w/v) was exposed to freshly collected buccal cells (ca. 48x10(4) cells/test) for 15 min at 30 degrees C. The cells were then rinsed with a small volume of double distilled water, allowed to air-dry on a freshy cleaved mica surface and imaged using contact mode AFM. Untreated cells showed relatively smooth surface characteristics, with many small 'crater-like' pits and indentations spread over cell surfaces. Cells that had been treated with all the investigated polymers appeared to have lost the crater and indentation characteristic and gained a higher surface roughness. These results suggest that polymer chains had adsorbed onto the cell surfaces. Quantitative image analysis of cell topography showed significant increases (P<0.05) in arithmetic roughness average (R(a)) for all the investigated polymer treated cells surfaces with respect to untreated control specimens. The changes in surface topography indicate the presence of adsorbed polymer, confirming previous work. This study demonstrates the suitability of AFM as a powerful and sensitive technique for detecting and imaging bioadhesive polymers present on mucosal cell surfaces.

Acrylic Resins↗

PubMed2002

Solid-state plasticization of an acrylic polymer with chlorpheniramine maleate and triethyl citrate.

The influence of in situ plasticization of chlorpheniramine maleate (CPM) on Eudragit RS PO from hot-melt extruded matrix tablets, and from compressed granules prepared by thermal processing was investigated. CPM was studied as both a model drug substance and as a solid-state plasticizer for the acrylic polymer. Triethyl citrate (TEC) was incorporated into the polymer blend as a liquid plasticizer for the polymer. The influence of TEC and CPM concentration on the dissolution properties of CPM tablets was investigated. The glass transition temperature (T(g)) of the samples was determined by modulated differential scanning calorimetry (MDSC). The morphologies of the granules formed by hot-melt extrusion and hot-melt granulation processes were investigated by scanning electron microscopy. The addition of 12% TEC to the polymer reduced the T(g) by 32.5 degrees C, while the reduction in the T(g) for the same level of CPM was 16.4 degrees C. The effect of TEC levels on drug release was dependent on the tablet preparation method. At high TEC levels, the release rate of CPM decreased in tablets prepared by direct compression and tablets made from compressed granules that had been prepared by high shear hot-melt granulation. However, the CPM release rate increased from hot-melt extruded tablets with increasing blends of plasticizer in the extruded tablets. An increase in the CPM content in the tablets resulted in an increase in the drug release rate. During high shear hot-melt granulation, the model drug adhered to the polymer to form a porous discontinuous structure. Following hot-melt extrusion, the drug was distributed at a molecular level in the continuous polymeric structure. The influence of both CPM and TEC levels on the drug release rate from these polymeric drug delivery systems was shown to be a function of whether the granules or tablets were formed by either hot-melt granulation or hot-melt extrusion, as well as the plasticization effects of both TEC and CPM on the acrylic polymer.

Chemistry, Pharmaceutical↗

PubMed2001

Effect of anionic polymers on the release of propranolol hydrochloride from matrix tablets.

Anionic polymers, namely Eudragit S, Eudragit L 100-55, and sodium carboxymethylcellulose, were incorporated into hydroxypropylmethylcellulose (HPMC K100M) to modify the drug release from HPMC matrices. The effects of changing the ratio of HPMC to anionic polymers were examined in water and in media with different pH. The dissolution profiles were compared according to release rates. The interaction between propranolol hydrochloride and anionic polymers was confirmed using the UV difference spectra method. The drug release was controlled with the type of anionic polymer and the interaction between propranolol hydrochloride and anionic polymers. The HPMC-anionic polymer ratio also influenced the drug release. The matrix containing HPMC-Eudragit L 100-55 (1:1 ratio) produced pH-independent extended-release tablets in water, 0.1 N HCl, and pH 6.8 phosphate buffer.

Acrylic Resins↗

PubMed2003

Dry polymer powder coating and comparison with conventional liquid-based coatings for Eudragit) RS, ethylcellulose and shellac.

Drug-layered pellets were coated with micronized polymer powders (Eudragit) RS, ethylcellulose, and shellac) by a dry powder coating technique as an alternative to organic- and aqueous-based coatings (Eudragit) RS 30D, Aquacoat) ECD) were investigated. High plasticizer concentrations (40%) and a thermal after-treatment (curing) were necessary for the coalescence of the polymer particles and good film formation. Ethylcellulose required a higher curing temperature and time than Eudragit) RS because of its higher glass transition temperature (133 versus 58 degrees C). A smaller polymer particle size also promoted film formation. In general, pellets coated with polymer powders required higher coating levels to obtain similar drug release patterns as pellets coated with organic polymer solutions and aqueous polymer dispersions.

Acrylic Resins↗

PubMed1994

Oxygen sensors based on luminescence quenching: interactions of metal complexes with the polymer supports.

Oxygen quenching of [Ru(Ph2phen)3]Cl2 (Ph2phen = 4,7-diphenyl-1,10-phenanthroline) has been studied in a diverse series of polymers, most with a common poly-(dimethylsiloxane) (PDMS) component. Systematic variations in the polymer properties have been made in order to delineate the structural features important for satisfactory use of supports for oxygen sensors. Most measurements were made using homo- or copolymers containing a PDMS region, although some measurements were made on small ring siloxane polymers. In particular, quenching behavior was examined as a function of polymer structure as well as the type of and amount of polar copolymer cross-linkers. Cross-linkers were added to enhance the solubility of oxygen probes in an otherwise nonpolar polymer. In addition, hydrophobic silica was added to alter quenching properties. Domain models are used to explain the variations in oxygen quenching properties as a function of additives and cross-linkers. These considerations have led to the most sensitive ruthenium-based sensor reported to date. The relative affinity of the different domains for the complex and the efficacy of the domains for oxygen quenching control the overall behavior of the sensing response. Guidelines for design of suitable polymer supports for oxygen sensors are proposed.

Acrylates↗

PubMed2001

Inverse least-squares modeling of vapor descriptors using polymer-coated surface acoustic wave sensor array responses.

In previous work, it was shown that, in principle, vapor descriptors could be derived from the responses of an array of polymer-coated acoustic wave devices. This new chemometric classification approach was based on polymer/vapor interactions following the well-established linear solvation energy relationships (LSERs) and the surface acoustic wave (SAW) transducers being mass sensitive. Mathematical derivations were included and were supported by simulations. In this work, an experimental data set of polymer-coated SAW vapor sensors is investigated. The data set includes 20 diverse polymers tested against 18 diverse organic vapors. It is shown that interfacial adsorption can influence the response behavior of sensors with nonpolar polymers in response to hydrogen-bonding vapors; however, in general, most sensor responses are related to vapor interactions with the polymers. It is also shown that polymer-coated SAW sensor responses can be empirically modeled with LSERs, deriving an LSER for each individual sensor based on its responses to the 18 vapors. Inverse least-squares methods are used to develop models that correlate and predict vapor descriptors from sensor array responses. Successful correlations can be developed by multiple linear regression (MLR), principal components regression (PCR), and partial least-squares (PLS) regression. MLR yields the best fits to the training data, however cross-validation shows that prediction of vapor descriptors for vapors not in the training set is significantly more successful using PCR or PLS. In addition, the optimal dimension of the PCR and PLS models supports the dimensionality of the LSER formulation and SAW response models.

Journal Article↗

PubMed1998

Stable capillary coating with successive multiple ionic polymer layers.

A stable modification of the inner wall of a fused silica capillary was established by a simple coating procedure, successive multiple ionic-polymer layer (SMIL) coating. An anionic polymer was tightly fixed to the capillary wall by the SMIL coating, in which a cationic polymer was sandwiched between the anionic polymer and the uncoated fused silica capillary by noncovalent bonding. The SMIL-coated capillary showed a long lifetime. The endurance of the SMIL-coated capillary was more than 100 runs, and it was also tolerant to organic solvents, 1 M NaOH, and a surfactant. The coating efficiency did not depend on capillary sources, and the relative standard deviation of capillary-to-capillary reproducibility was less than 1%. In this study, dextran sulfate (DS) was used as the anionic polymer, and Polybrene was used as the cationic polymer for SMIL modification. The DS-modified capillary (SMIL-DS capillary) exhibited a pH-independent electroosmotic flow (EOF) from anode to cathode in the pH range of 2-11. The SMIL-DS capillary showed good performance for acidic protein analyses under physiological conditions (pH 7.4). Also, the presence of EOF under acidic conditions permitted new applications. Simultaneous separations of cationic, anionic, and neutral amino acids were achieved by capillary zone electrophoresis, and separations of cresol isomers were achieved by micellar electrokinetic chromatography under the acidic conditions. The SMIL-DS capillary was also useful for fast and precise determination of the pKa of acidic functional groups.

Amino Acids↗