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PubMed2001

Membrane curvature induced by polymer adsorption.

The phenomena resulting from interaction between polymers and membranes pose important problems for biological applications. Based on a scaling theory, we investigate the spontaneous curvature of a membrane induced by either flexible or semiflexible chain adsorption. Irrespective of chain stiffness, a weakly adsorbed polymer induces the membrane to bend away (to have a positive curvature) from the polymer mostly due to increase of the conformational entropy compared with that for a flat surface. On the other hand, a strongly adsorbed polymer induces the membrane to bend toward the polymer mostly due to decrease in the interaction energy, leading to a possibility of encapsulation of polymer by the membrane.

Adsorption↗

PubMed2005

Elasticity of polymer vesicles by osmotic pressure: an intermediate theory between fluid membranes and solid shells.

The entropy of a polymer confined in a curved surface and the elastic free energy of a membrane consisting of polymers are obtained by scaling analysis. It is found that the elastic free energy of the membrane has the form of the in-plane strain energy plus Helfrich's curvature energy [Z. Naturforsch. C 28, 693 (1973)]. The elastic constants in the free energy are obtained by discussing two simplified models: one is the polymer membrane without in-plane strains and asymmetry between its two sides, which is the counterpart of quantum mechanics in a curved surface [H. Jensen and H. Koppe, Ann. Phys. (N.Y) 63, 586 (1971)]; the other is the planar rubber membrane with homogeneous in-plane strains. The equations to describe equilibrium shape and in-plane strains of the polymer vesicles by osmotic pressure are derived by taking the first-order variation of the total free energy containing the elastic free energy, the surface tension energy, and the term induced by osmotic pressure. The critical pressure above which a spherical polymer vesicle will lose its stability is obtained by taking the second-order variation of the total free energy. It is found that the in-plane mode also plays an important role in the critical pressure because it couples with the out-of-plane mode. Theoretical results reveal that polymer vesicles possess mechanical properties intermediate between those of fluid membranes and solid shells.

Computer Simulation↗

PubMed2003

Entropic phase separation in polymer-microemulsion networks.

We study theoretically a model system of a transient network of microemulsion droplets connected by telechelic polymers and explain recent experimental findings. Despite the absence of any specific interactions between either the droplets or polymer chains, we predict that as the number of polymers per drop is increased, the system undergoes a first-order phase separation into a dense, highly connected phase, in equilibrium with dilute droplets, decorated by polymer loops. The phase transition is purely entropic and is driven by the interplay between the translational entropy of the drops and the configurational entropy of the polymer connections between them. Because it is dominated by entropic effects, the phase behavior of the system is extremely robust and is independent of the detailed properties of either polymers or drops.

Emulsions↗

PubMed2006

Polymer packaging and ejection in viral capsids: shape matters.

We use a mesoscale simulation approach to explore the impact of different capsid geometries on the packaging and ejection dynamics of polymers of different flexibility. We find that both packing and ejection times are faster for flexible polymers. For such polymers a sphere packs more quickly and ejects more slowly than an ellipsoid. For semiflexible polymers, however, the case relevant to DNA, a sphere both packs and ejects more easily. We interpret our results by considering both the thermodynamics and the relaxational dynamics of the polymers. The predictions could be tested with biomimetic experiments with synthetic polymers inside artificial vesicles. Our results suggest that phages may have evolved to be roughly spherical in shape to optimize the speed of genome ejection, which is the first stage in infection.

Capsid↗

PubMed2004

Hydrated metal(II) complexes of N-(6-amino-3,4-dihydro-3-methyl-5-nitroso-4-oxopyrimidin-2-yl) derivatives of glycine, glycylglycine, threonine, serine, valine and methionine: a monomeric complex and coordination polymers in one, two and three dimensions linked by hydrogen bonding.

Nine hydrated complexes of Group 2 (alkaline earth) cations with organic ligands which are N-substituted amino acids containing the 6-amino-3,4-dihydro-3-methyl-5-nitroso-4-oxopyrimidin-2-yl group have been structurally characterized. The octahydrated calcium glycinate complex, where the six-coordinate Ca cation lies on an inversion centre in the space group P(-)1, forms a finite (zero-dimensional) complex. The hexahydrated barium glycinate complex contains eight-coordinate Ba and it is isostructural with the known Sr analogue, and its one-dimensional coordination polymer takes the form of a simple chain. The octahydrated calcium and strontium threonine complexes are isostructural, with eight-coordinate cations lying on twofold rotation axes in the space group C2: the one-dimensional coordination polymers take the form of a chain of spiro-fused rings and a similar chain of spiro-fused rings is found in the heptahydrated barium serine complex, although here the ten-coordinate cation lies in a general position. In the tetrahydrated strontium and barium glycylglycinate complexes, the eight-coordinate cations lie on twofold rotation axes in the space group C2/c, but in the Sr complex the coordination polymer is a chain of spiro-fused rings, while in the Ba complex the coordination polymer forms deeply puckered sheets. There are two types of Ca site in the hexahydrated calcium valine complex: one is eight coordinate and gives rise to a two-dimensional coordination polymer, while the other is seven coordinate forming a finite, zero-dimensional coordination complex. In the heptahydrated barium methionine complex, the coordination polymer is three dimensional. In all of the complexes, the coordination aggregates are further linked by an extensive series of hydrogen bonds.

Amino Acids↗

PubMed1977

The effect of various metal ions and chelating agents on the formation of noncovalently and covalently linked IgM polymers.

The influence of various concentrations of Mg2+, Ca2+, Mn2+, Fe2+, Fe3+, Co2+, Ni2+, Cu2+, Zn2+, Cd2+, Hg2+, EDTA, or 8-hydroxyquinoline-5-sulfonic acid on the formation in vitro of polymeric IgM from reduced and dissociated IgM has been investigated. 4-200muM Zn, Cd, or Hg ions in the dialysis buffer used for reassociation resulted in the formation of a homogeneous polymer peak sedimenting as 19S IgM, whereas the other metal ions resulted in the formation of polymers sedimenting mostly as tetramers, pentamers (19S IgM), and hexamers. Dialysis in the presence of 1 and 3mM EDTA or 8-hydroxyquinoline-5-sulfonic acid gave slight polymer formation; 10 mM of the agents gave none. Ca, Mg, Fe, Ni, Zn, Cd, or Hg ions regularly gave only noncovalently linked polymers, whereas Cu ions in particular, but also Co and, to a minor extent, Mn ions catalyzed the formation of covalently linked polymers. Experiments performed with Mg, Ca, Ni, and Zn ions or with Cu and Zn ions in the same buffer during reassociation showed that Zn ions inhibit the effect of the other ions on polymer assembly and covalent stabilization.

Chelating Agents↗

PubMed1994

Chiral recognition of N alpha-protected amino acids and derivatives in non-covalently molecularly imprinted polymers.

Highly crosslinked synthetic polymers, selective for various N alpha-protected amino acids and derivatives, were prepared by non-covalent molecular imprinting. Methacrylic acid and ethylene glycol dimethacrylate were copolymerized in the presence of the print molecules, which were subsequently extracted from the polymers. The recognition of the polymers for the print molecules and molecules of similar structures was investigated by using the polymers as stationary phases in HPLC. The functional groups of the print molecules interact via hydrogen bonds with the positioned carboxyls of the polymer. It was shown that the N alpha-protecting group, the C alpha-protecting group and the amino acid side chain are also recognized by the binding sites in the polymer.

Amino Acids↗

PubMed1985

Use of tyrosine-containing polymers to characterize the substrate specificity of insulin and other hormone-stimulated tyrosine kinases.

Synthetic copolymers containing tyrosine residues were used to characterize the substrate specificity of the insulin receptor kinase and compare it to tyrosine kinases stimulated by epidermal growth factor, insulin-like growth factor-1 and phorbol ester. In partially purified receptor preparations from eight different tissues insulin best stimulated (highest V) phosphorylation of a random copolymer composed of glutamic and tyrosine residues at a 4:1 ratio (Glu/Tyr, 4:1). The insulin-stimulated phosphorylation of this polymer was highly significant also in receptor preparations from fresh human monocytes, where insulin binding and autophosphorylation were difficult to detect. Other tyrosine-containing polymers Ala/Glu/Lys/Tyr (6:2:5:1) and Glu/Ala/Tyr (6:3:1) were also phosphorylated by the insulin-stimulated kinase but to a lower extent. A tyrosine kinase stimulated by insulin-like growth factor-1, and one stimulated by phorbol ester also best phosphorylated the polymer Glu/Tyr (4:1). The three kinases differed only in their capability to phosphorylate Glu/Ala/Tyr (6:3:1) or Ala/Glu/Lys/Tyr (6:2:5:1). Glu/Tyr (4:1) was a poor substrate for the epidermal growth factor receptor kinase which best phosphorylated the polymer Glu/Ala/Tyr (6:3:1). Three additional polymers: Glu/Tyr (1:1), Glu/Ala/Tyr (1:1:1), and Lys/Tyr (1:1) failed to serve as substrates for all four tyrosine kinases tested. Taken together these findings suggest that. Hormone-sensitive tyrosine kinases have similar yet distinct substrate specificity and are likely to phosphorylate their native substrates on tyrosines adjacent to acidic (glutamic) residues. Tyrosine-containing polymer substrates are highly sensitive and convenient tools to study (hormone-sensitive) tyrosine kinases whose native substrates are unknown or present at low concentrations.

Animals↗

PubMed1995

"Intelligent" polymers in medicine and biotechnology.

One can define "intelligent" polymers as those polymers that respond with large property changes to small physical or chemical stimuli. These polymers may be in various forms, such as in solution, on surfaces, or as solids. One may also combine intelligent aqueous polymer systems with biomolecules to yield a large family of polymers that respond intelligently to physical, chemical, or biological stimuli. This article overviews such interesting and versatile polymer systems.

Biochemical Phenomena↗

PubMed1992

Biodegradability of polymers in the environment: complexities and significance of definitions and measurements.

There is a world-wide research effort to develop biodegradable polymers as a waste-management option for polymers in the environment. This effort may prove to be fruitless unless we can agree on a definition and test protocols--what do we expect biodegradable polymers to do in the environment and how do we demonstrate that they do what we expect? Establishing a definition and test protocols is not trivial; the task is made complex by the wide range of disciplines involved directly in or interested in the subject, including polymer scientists, biochemists, environmentalists, legislators, and laypeople, all with their own perspectives and expectations. In this paper, I present arguments in favor of biodegradable polymers and indicate what remains to be done to satisfy detractors that they represent a viable option for polymer waste-management.

Biodegradation, Environmental↗

PubMed2005

Radiological properties of normoxic polymer gel dosimeters.

The radiological properties of the normoxic polymer gel dosimeters MAGIC, MAGAS, and MAGAT [methacrylic and ascorbic acid in gelatin initiated by copper; methacrylic acid gelatine gel with ascorbic acid; and methacrylic acid gelatine and tetrakis (hydroxymethyl) phosphonium chloride, respectively] have been investigated. The radiological water equivalence was determined by comparing the polymer gel macroscopic photon and electron interaction cross sections over the energy range from 10 keV to 20 MeV and by Monte Carlo modeling of depth doses. Normoxic polymer gel dosimeters have a high gelatine and monomer concentration and therefore mass density (kg m(-3)) up to 3.8% higher than water. This results in differences between the cross-section ratios of the normoxic polymer gels and water of up to 3% for the attenuation, energy absorption, and collision stopping power coefficient ratios through the Compton dominant energy range. The mass cross-section ratios were within 2% of water except for the mass attenuation and energy absorption coefficients ratios, which showed differences with water of up to 6% for energies less than 100 keV. Monte Carlo modeling was undertaken for the polymer gel dosimeters to model the electron and photon transport resulting from a 6 MV photon beam. The absolute percentage differences between gel and water were within 1% and the relative percentage differences were within 3.5%. The results show that the MAGAT gel formulation is the most radiological water equivalent of the normoxic polymer gel dosimeters investigated due to its lower mass density measurement compared with MAGAS and MAGIC gels.

Ascorbic Acid↗

PubMed1994

Functional polymers and dendrimers: reactivity, molecular architecture, and interfacial energy.

The interaction of polymers with their environment depends largely on the functional groups they carry. Interfaces between different polymers or between polymers and other surfaces can be strengthened through the design of molecular interactions such as hydrogen bonding and through the control of polymer architecture. The placement of functional groups at polymer chain ends or in well-defined segments can determine the ultimate properties. Three-dimensional synthetic polymers such as dendrimers can be fashioned to encapsulate reactive sites or provide highly controlled surfaces and interfaces.

Hydrogen Bonding↗

PubMed1999

Bacterial cell wall polymers promote intestinal fibrosis by direct stimulation of myofibroblasts.

Normal luminal bacteria and bacterial cell wall polymers are implicated in the pathogenesis of chronic intestinal inflammation. To determine the direct involvement of bacteria and their products on intestinal fibrogenesis, the effects of purified bacterial cell wall polymers on collagen and cytokine synthesis were evaluated in intestinal myofibroblast cultures established from normal fetal and chronically inflamed cecal tissues. In this study, the intestines of Lewis rats were intramurally injected with peptidoglycan-polysaccharide polymers. Collagen and transforming growth factor (TGF)-beta1 mRNA levels were measured and correlated with mesenchymal cell accumulation by immunohistochemistry. The direct effects of cell wall polymers on fibrogenic cytokine and collagen alpha1 (type I) expression were evaluated in intestinal myofibroblast cultures. We found that intramural injections of bacterial cell wall polymers induced chronic granulomatous enterocolitis with markedly increased collagen synthesis and concomitant increased TGF-beta1 and interleukin (IL)-6 expression. Intestinal myofibroblast cultures were established, which both phenotypically and functionally resemble the mesenchymal cells that are involved in fibrosis in vivo. Bacterial cell wall polymers directly stimulated collagen alpha1 (I), TGF-beta1, IL-1beta, and IL-6 mRNA expression in the intestinal myofibroblasts derived from both normal and inflamed cecum. Neutralization of endogenous TGF-beta1 inhibited in vitro collagen gene expression. From our results, we conclude that increased exposure to luminal bacterial products can directly activate intestinal mesenchymal cells, which accumulate in areas of chronic intestinal inflammation, thus stimulating intestinal fibrosis in genetically susceptible hosts.

Animals↗

PubMedDate not supplied

Topical application of ionic polymers affects skin permeability barrier homeostasis.

We previously demonstrated that the external electric potential affected skin barrier homeostasis. On the other hand, topical application of an ionic polymer formed a diffusion electric double layer on the surface of the skin. Thus, we evaluated effects of topical application of ionic polymers on the damaged skin barrier. Application of a nonionic polymer did not affect barrier recovery. Application of sodium salts of anionic polymers accelerated barrier recovery, while that of cationic polymers delayed it. Topical application of a sodium-exchange resin accelerated barrier recovery, but application of a calcium-exchange resin had no effect even when the resins had the same structure. Application of a chloride-exchange resin delayed barrier recovery. Topical application of ionic polymers influenced skin barrier homeostasis.

Administration, Cutaneous↗

PubMed1976

Ampicillin polymers as elicitors of passive cutaneous anaphylaxis.

The ability of ampicillin polymers to elicit passive cutaneous anaphylaxis (PCA) reactions in guinea pigs was analyzed. Mediating antibodies were raised in rabbits against a crude preparation of 6-aminopenicillanic acid (6-APA). It was found that large ampicillin polymers were potent elicitors, 1,000-fold better than benzylpenicillin polymers. Small polymers in high concentrations did not elicit PCA reactions but inhibited the activity of the larger polymers. This inhibition was more pronounced that that of ampicillin monomer. High molecular weight of ampicillin polymer in the amount of 0.1% in an ampicillin solution manifested its PCA activity. The tendency of ampicillin to polymerize, particularly when kept in solution, makes this observation worth considering. The PCA reactions described were penicilloyl-specific as verified by immunosorbent experiments.

Ampicillin↗

PubMed1987

Increased plasma concentration of cross-linked fibrin polymers in acute myocardial infarction.

Thrombin cleaves fibrinopeptides from fibrinogen, converting it to fibrin monomer, and activates factor XIII, which catalyzes the formation of intermolecular epsilon-(gamma-glutamyl)-lysine bonds to stabilize the fibrin polymer. The formation of factor XIIIa-catalyzed fibrin polymers during clotting of plasma and purified fibrinogen in vivo was followed by a sodium dodecyl sulfate agarose gel technique, and an increase in both amount and size of gamma-chain cross-linked polymers was demonstrated before visible clot formation. Plasma from patients presenting with acute myocardial infarction showed increases in the plasma concentration of fibrin polymer and in the proportion of total fibrinogen present as polymer, as determined by a quantitative adaptation of the electrophoretic technique. The plasma concentration in patients with subendocardial or transmural myocardial infarction showed significant (p less than .005) increases to 4.0 +/- 1.0% and 3.6 +/- .8%, respectively, as compared with the concentration in normal plasma (0.8 +/- 0.1%). There was no difference in plasma concentration in samples from patients with transmural compared with those with subendocardial myocardial infarction. This study provides the first demonstration of factor XIIIa cross-linked fibrin polymers in thrombotic disease and indicates the presence of increased activity of both thrombin and factor XIIIa in patients with acute myocardial infarction.

Blood Coagulation↗

PubMed2003

Modification of porous aminopropyl-silicate microcapsule membrane by electrically-bonded external anionic polymers.

Biocompatibility and permeability of a microcapsule membrane governs the function of a microcapsule-shaped bioartificial pancreas. We have previously developed an alginate/sol-gel-synthesized aminopropyl-silicate/alginate microcapsule (Alg/AS/Alg), which had insufficient biocompatibility. The purpose of this study was to investigate whether the biocompatibility could improve by modifying the external surface with other anionic polymers and to investigate an influence of the modification on the permeability of the membrane. Four kinds of anionic polymers, poly(oxyethylene)diglycolic acid (3 kDa), heparin (15 kDa), Alg (54 kDa) and carboxymethylcellulose (CMC, 60 kDa) were used as the external anionic polymers. The heparin-bonded gel bead had the largest resistance to the diffusion of small molecules. The molecular mass cut-off point of 150 kDa required for immunoisolation was maintained for all anionic polymers. Cellular overgrowth to the implanted islet-enclosing microcapsule, a sign of insufficient biocompatibility, was suppressed by altering the external surface material from Alg to CMC. These results suggest that the biocompatibility of the Alg/AS/anionic polymer membrane can be improved by using a biocompatible anionic polymer. At the same time, it is suggested the influence on the permeability has to be investigated to develop an optimal microcapsule for bioartificial pancreas.

Animals↗

PubMed2005

Microwave-assisted synthesis of poly(epsilon-caprolactone)-poly(ethylene glycol)-poly(epsilon-caprolactone) tri-block co-polymers and use as matrices for sustained delivery of ibuprofen taken as model drug.

Poly(epsilon-caprolactone)-poly(ethylene glycol)-poly(epsilon-caprolactone) triblock co-polymers with number-average molar mass (Mn) over 20000 g/mol were prepared by ring-opening polymerization of epsilon-caprolactone initiated by poly(ethylene glycol) under microwave irradiation. This method was proposed as a means to improve in vivo compatibility as no harmful chemicals were involved in the polymerization except epsilon-caprolactone and poly(ethylene glycol). The resulting tri-block co-polymers were characterized by FT-IR, H-NMR, GPC and WAXD. Their Mn and their composition was controlled by the amount and the chain length of the poly(ethylene glycol) macromers involved in the feed. The ability of poly(epsilon-caprolactone)-poly(ethylene glycol)-poly(epsilon-caprolactone) co-polymers to entrap and deliver drugs was investigated with ibuprofen as a model drug. The release of ibuprofen was significantly influenced by the co-polymer composition and the extent of loading. The in vitro release of ibuprofen was sustained from 3 to 15 days for 10% loading, depending on the ratio of epsilon-caprolactone to ethylene glycol-derived subunits in co-polymer chains. This ratio ranged from 0.97 to 9.78. In the case of the co-polymer whose epsilon-caprolactone molar ratio to ethylene glycol-derived subunits was 2.49, the ibuprofen release was sustained for 2 to 24 days for ibuprofen loads going from 5 to 20 wt%.

Drug Delivery Systems↗