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PubMedDate not supplied

In vitro and in vivo evaluation of hydrophilic dendronized linear polymers.

Rigid-rod dendronized linear polymers consisting of a poly(4-hydroxystyrene) backbone and fourth-generation polyester dendrons were evaluated in vitro and in vivo to determine their suitability as drug delivery vectors. Cytotoxicity assays indicated that the polymers were well tolerated by cells in vitro. Biodistribution studies of the polymers in both nontumored and tumored mice revealed that as for random coil linear polymers, renal clearance was a function of polymer size, with significant urinary excretion observed for a 67 kDa dendronized polymer. High accumulation in organs of the reticuloendothelial system was exhibited by a dendronized polymer with a very high molecular weight (M(n) = 1740 kDa), but was not as significant for smaller polymers with M(n) = 67 kDa and M(n) = 251 kDa. The rank order for tumor accumulation of the polymers on a percent injected dose per gram tumor basis was 251 kDa approximately 1740 kDa > 67 kDa. These data will help guide the selection of highly functionalizable rigid-rod dendronized polymers with pharmacokinetic properties appropriate for use as drug carriers.

Animals↗

PubMedDate not supplied

Polyelectrolyte vectors for gene delivery: influence of cationic polymer on biophysical properties of complexes formed with DNA.

Cationic polymer/DNA complexes are widely used for gene delivery, although the influence of the cationic polymer on the biophysical properties of the resulting complex is poorly understood. Here, several series of cationic polymers have been used to evaluate the influence of structural parameters on properties of DNA complexes. Parameters studied included the length of side chain, charge type (primary versus tertiary and quaternary), polymer molecular weight, and charge spacing along the polymer backbone. Cationic polymers with short side chains (such as polyvinylamine) formed small complexes, resistant to destabilization by polyanions, with low surface charge, limited transfection activity, and efficient intranuclear transcription. Conversely, cationic polymers with long side chains (e.g., poly[methacryloyl-Gly-Gly-NH-(CH(2))(6)-NH(2))] showed inefficient complex formation, high positive surface charge, and better transfection activity. The effects of molecular weight varied between polymers, for example, low molecular weight poly(L-lysine) produced relatively small complexes, whereas low molecular weight poly[2-(trimethylammonio)ethyl methacrylate chloride] produced large aggregates. Polymers containing quaternary ammonium groups showed efficient complex formation but poor transfection. Finally, spreading charges widely on the polymer structure inhibited their ability to condense DNA. In summary, to achieve small, stable complexes, the use of cationic polymers with short side chains bearing primary amino groups is suggested.

Animals↗

PubMedDate not supplied

Cloning strategy for producing brush-forming protein-based polymers.

Brush-forming polymers are being used in a variety of applications, and by using recombinant DNA technology, there exists the potential to produce protein-based polymers that incorporate unique structures and functions in these brush layers. Despite this potential, production of protein-based brush-forming polymers is not routinely performed. For the design and production of new protein-based polymers with optimal brush-forming properties, it would be desirable to have a cloning strategy that allows an iterative approach wherein the protein based-polymer product can be produced and evaluated, and then if necessary, it can be sequentially modified in a controlled manner to obtain optimal surface density and brush extension. In this work, we report on the development of a cloning strategy intended for the production of protein-based brush-forming polymers. This strategy is based on the assembly of modules of DNA that encode for blocks of protein-based polymers into a commercially available expression vector; there is no need for custom-modified vectors and no need for intermediate cloning vectors. Additionally, because the design of new protein-based biopolymers can be an iterative process, our method enables sequential modification of a protein-based polymer product. With at least 21 bacterial expression vectors and 11 yeast expression vectors compatible with this strategy, there are a number of options available for production of protein-based polymers. It is our intent that this strategy will aid in advancing the production of protein-based brush-forming polymers.

Amino Acid Sequence↗

PubMed2002

Use of polymer mats in series for sequential reactive barrier remediation of ammonium-contaminated groundwater: laboratory column evaluation.

Large-scale column experiments were undertaken to evaluate the potential of in situ polymer mats (installed in series) to be used as permeable reactive barriers for delivery of oxidants and reductants to induce sequential bioremediation of ammonium-contaminated groundwater (approximately 120mg L(-1) NH4+-N), without bioaugmentation. The strategy was for the first group of polymer mats to deliver oxygen to induce bacterial nitrification of the ammonium to nitrite/ nitrate as the groundwater moved past and for the second group of polymer mats to deliver hydrogen or ethanol, to induce bacterial denitrification of the nitrite/nitrate to produce nitrogen gas. Once purging of the first polymer mat commenced, ammonium concentrations decreased downgradient from the polymer mats. Nitrification rates increased and stabilized over the 6-month experiment, with stable nitrification half-lives in the range 0.07-0.25 days. Nitrification most likely occurred in a biologically active zone at the polymer wall/aqueous interface. With hydrogen delivery via the polymer mats, a denitrification half-life (nitrate plus nitrite removal) of 3.5 days was induced. Denitrification rates were significantly enhanced when ethanol was delivered via a polymer mat, with denitrification half-lives in the range of 0.12-0.34 days. Nitrification/ denitrification rates were maintained for groundwater flow rates up to 300 m yr(-1), suggesting oxygen and ethanol delivery rates via the polymer mats were sufficient not to limit nitrification or denitrification. In soil columns, the polymer mat delivery system provided an effective and reliable technique for delivery of oxygen and hydrogen or ethanol for sequential nitrification/denitrification of ammonium-contaminated groundwater. Scale-up of this concept to a field pilot-scale is currently underway.

Biodegradation, Environmental↗

PubMed2005

Solid-phase synthesis of polymers using the ring-opening metathesis polymerization.

We report a general method for the solid-phase synthesis of polymers via the ring-opening metathesis polymerization (ROMP). The method involves polymerization in solution to form a block copolymer, immobilization of the polymer via reaction of one block with a resin-bound functional group, modification of the other block, and liberation of the polymer from the resin. We demonstrated the utility of this approach by generating a block copolymer with an N-hydroxysuccinimidyl ester-substituted block (for on-resin functionalization) and a maleimide-substituted block (for conjugation to the resin). We showed that the Diels-Alder reaction can be employed to immobilize the polymers and that amines of diverse structure can be used to modify the resin-bound polymers. The reversibility of the furan-maleimide Diels-Alder adduct was exploited to liberate the polymer from the support. Specifically, treatment of the resin with cyclopentadiene resulted in complete polymer release. The resulting polymers are functional: they were as potent in assays with the lectin concanavalin A as polymers generated by traditional solution routes. We anticipate that this method can be used for the rapid synthesis of diverse polymers via ROMP.

Esters↗

PubMed2005

Synthesis of functionalized asymmetric star polymers containing conductive polyacetylene segments by living anionic polymerization.

Novel 3-arm ABC, 4-arm ABCD, and 5-arm ABCDE asymmetric star polymers comprising the conductive polyacetylene precursor, poly(4-methylphenyl vinyl sulfoxide) (PMePVSO), and other segments, such as polystyrene, poly(alpha-methylstyrene), poly(4-methoxystyrene), poly(4-trimethylsilylstyrene), and poly(4-methylstyrene), were synthesized by the methodology based on living anionic polymerization using DPE-functionalized polymers. This methodology involves the addition reaction of a DPE-functionalized polymer to a living anionic polymer followed by the living anionic polymerization of MePVSO initiated from the in situ formed polymer anion with two, three, or four polymer segments. The resultant asymmetric star polymers possessed predetermined molecular weights, narrow molecular weight distributions (Mw/Mn < 1.03), and desired compositions as confirmed by SEC, 1H NMR, SLS, and elemental analysis. After thermal treatment, the PMePVSO segment in the star polymer could be completely converted into a conductive polyacetylene segment, evident from TGA and elemental analysis. These asymmetric star polymers are expected to exhibit interesting solution properties and unique microphase-separated morphological suprastructures with potential applications in nanoscopic conductive materials. Moreover, this methodology can afford the target asymmetric star polymers with arm segments varying in a wide range and enables the synthesis of more complex macromolecular architectures.

Acetylene↗

PubMed2006

Phase biaxiality in nematic liquid crystalline side-chain polymers of various chemical constitutions.

In a previous deuterium NMR study conducted on a liquid crystalline (LC) polymer with laterally attached book-shaped molecules as the mesogenic moiety, we have revealed a biaxial nematic phase below the conventional uniaxial nematic phase (Phys. Rev. Lett. 2004, 92, 125501). To elucidate details of its formation, we here report on deuterium NMR experiments that have been conducted on different types of LC side-chain polymers as well as on mixtures with low-molar-mass mesogens. Different parameters that affect the formation of a biaxial nematic phase, such as the geometry of the attachment, the spacer length between the polymer backbone and the mesogenic unit, as well as the polymer dynamics, were investigated. Surprisingly, also polymers with terminally attached mesogens (end-on polymers) are capable of forming biaxial nematic phases if the flexible spacer is short and thus retains a coupling between the polymer backbone and the LC phase. Furthermore, the most important parameter for the formation of a biaxial nematic phase is the dynamics of the polymer backbone, as the addition of a small percentage of low molar mass LC to the biaxial nematic polymer from the original study served to shift both the glass transition and the appearance of detectable biaxiality in a very similar fashion. Plotting different parameters for the investigated systems as a function of T/Tg also reveals the crucial role of the dynamics of the polymer backbone and hence the glass transition.

Crystallization↗

PubMed2005

Depletion and pair interactions of proteins in polymer solutions.

We study the depletion, pair interaction, and phase behavioral characteristics of proteins in polymer solutions. We use a McMillan-Mayer-like approach [W. G. McMillan, Jr. and J. E. Mayer, J. Chem. Phys. 13, 276 (1945)] to suggest that the depletion characteristics should be studied at an effective polymer concentration which is a function of both the average polymer and the protein concentrations. In the protein limit, we show that the volume of the polymer depletion layers exceeds the size of the proteins, leading to effective polymer concentrations typically in the semidilute and concentrated regimes even when the average polymer concentrations are in the dilute regimes. We propose an approximate approach that accounts for the multibody depletion overlaps, and use an accurate numerical solution of polymer mean-field theory to address depletion characteristics in these regimes which are characterized by both the importance of polymer interactions as well as the curvature of the proteins relative to the correlation length of polymers. We show that the depletion characteristics of the protein-polymer mixture can be quite different when viewed in this framework, and this can have profound consequences for the phase behavior of the mixture. Our theoretical predictions for the phase diagram match semiquantitatively with published experimental results.

Biophysical Phenomena↗

PubMed2007

Synthesis and evaluation of molecularly imprinted polymers as sorbents of moniliformin.

Moniliformin is a low molecular weight mycotoxin that has worldwide potential to contaminate cereal grains. Although several traditional methods have been developed to detect moniliformin, the lack of anti-moniliformin antibodies has created a need for materials that recognize moniliformin at the molecular level through a binding mechanism. To address this issue, the authors synthesized molecularly imprinted polymers that bind moniliformin. Imprinted and non-imprinted polymers were evaluated by equilibrium binding assays and moniliformin concentrations were measured by LC analysis using ultraviolet light detection. Successful polymers were imprinted with toxin analogues as the templates; non-imprinted polymers exhibited minimal binding in acetonitrile under the assay conditions. Selected imprinted polymers also bound moniliformin in ethanol, methanol and dimethyl formamide. Significant differences in moniliformin binding by the polymers were dependent on polymer composition, and these differences were highly dependent on the template used to imprint the polymer. Polymers were further evaluated as sorbents for molecularly imprinted solid-phase extraction (MISPE), and an imprinted polymer was used for preconcentration and clean-up of a moniliformin spiked corn extract.

Chromatography, Liquid↗

PubMedDate not supplied

Effect of manufacturing conditions on the formation of double-walled polymer microspheres.

This paper discusses the optimization of the solvent evaporation process to produce double-walled (DW) microspheres in a single-step. Five process variables were studied: polymer solution concentration, polymer weight ratio, polymer solution volume ratios, encapsulation temperature, and air flow rate across the top of the encapsulation vessel. The effects of these variables on the process efficiency (defined here as the percentage of microspheres with a DW configuration compared to the total number of microspheres) were examined. Total polymer concentrations of less than 20% (w/v) produced microspheres with high efficiency, with phase separation consistent across all size fractions in each batch. Changing the volume ratio of the two polymer solutions had no significant effect on the process efficiency. The weight ratio of the polymers greatly influenced the process efficiency, resulting in a low 63% efficiency for the 1:3 Poly-L-lactide (PLLA): Poly(carboxyphenoxypropane-co-sebacic)anhydride 20:80 (P(CPP:SA 20:80)) weight ratio and 0% for the 3:1 weight ratio. The 1:3 weight ratio also caused the polymers to reverse their orientation, although the efficiency for this switch was still relatively low. The temperature of the non-solvent bath affected the efficiency of certain pairs of polymers, but not all. The PLLA/Poly(lactide-co-glycolide) 50:50 (PLGA) pair was most sensitive to temperature, due to the chemical similarity of the two polymers which narrowed the range of acceptable conditions for encapsulation. Pairs of polymers which phase separated readily (e.g. polystyrene and PLLA) were the least sensitive to temperature changes. Process yield and size distribution show no clear trends with respect to air flow rate across the top of the reaction vessel. The efficiency of the process to produce DW microspheres increased and the process time decreased with increasing air flow across the surface of the encapsulation vessel.

Chemistry, Pharmaceutical↗

PubMed1956

Efficiency of glutamyl peptide polymers as plasma volume extenders.

A series of polymers of polyglutamic acid have been tested as plasma volume expanders. The results indicate that those polymers prepared from backbones of 40,000 molecular weight or over and side chains of 3,000 molecular weight or over, will have plasma volume retention half-life of 15 hours or longer. Measurements of the oncotic efficiency of these polymers in vivo indicated a blood stream fluid retention of approximately 51 ml./gm. of polymer. Similar measurements of polymer-serum albumin solutions in vitro showed a retention of 52 ml./gm. of polymer. The clinical response to infusion of solutions of these polymers indicated no untoward pharmacological properties. Although the number of trials presented is too small for ultimate conclusion regarding either the physiological or clinical effects of these polymers, they do provide a strong indication of the desirability of further clinical testing of this polymer and a sound basis on which to plan the larger scale preparation of polymer. Both measures are currently under way.

Glutamates↗

PubMed1962

Effects of silicate polymers on erythrocytes in presence and absence of complement.

The effects of silicates upon erythrocytes depend upon the degree of polymerization. Monomeric silicate does not appear to be taken up by red cells. Polymerized silicates are taken up and bound tightly. In the presence of small polymeric forms erythrocytes are lysed by complement. Larger polymers are bound to erythrocytes but do not sensitize to complement hemolysis. Larger polymers, however, are directly toxic and cause hemolysis in the absence of complement. Red cells exposed to complement-active polymers show characteristic alteration in morphology with the assumption of irregular bell shapes. Larger polymers cause the cells to become spherical before spontaneous rupture occurs. Large polymers cause erythrocyte agglutination but this is minimal or absent with small complement-active polymers. Complement-active polymers cause little or no change in osmotic fragility. Increase in mechanical fragility is a sensitive indication of the presence of larger, agglutinating polymers. The conversion of pneumococci from Gram positivity to negativity appears to be caused principally by complement-active polymers. Possible implications of polymer size and complement activity are discussed in relation to production of silicotic lesions by silica-containing ores.

Complement System Proteins↗

PubMed2006

Polymer property prediction and optimization using neural networks.

Prediction and optimization of polymer properties is a complex and highly nonlinear problem with no easy method to predict polymer properties directly and accurately. The problem is especially complicated with high molecular weight polymers such as engineering plastics which have the greatest use in industry. The effect of modifying a monomer (polymer repeat unit) on polymerization and the resulting polymer properties is not easy to investigate experimentally given the large number of possible changes. This severely curtails the design of new polymers with specific end-use properties. In this paper, we show how properties of modified monomers can be predicted using neural networks. We utilize a database of polymer properties and employ a variety of networks ranging from backpropagation networks to unsupervised self-associating maps. We select particular networks that accurately predict specific polymer properties. These networks are classified into groups that range from those that provide quick training to those that provide excellent generalization. We also show how the available polymer database can be used to accurately predict and optimize polymer properties.

Forecasting↗

PubMed1989

Response of microbial adhesives and biofilm matrix polymers to chemical treatments as determined by interference reflection microscopy and light section microscopy.

The polymers involved in the adhesion of Pseudomonas fluorescens H2S to solid surfaces were investigated to determine whether differences between cell surface adhesives and biofilm matrix polymers could be detected. Two optical techniques, i.e., interference reflection microscopy (IRM) and light section microscopy (LSM), were used to compare the responses of the two types of polymer to treatment with electrolytes, dimethyl sulfoxide (DMSO), and Tween 20. To evaluate initial adhesive polymers, P. fluorescens H2S cells were allowed to attach to glass cover slip surfaces and were immediately examined with IRM, and their response to chemical solutions was tested. With IRM, changes in cell-substratum separation distance between 0 and ca. 100 nm are detectable as changes in relative light intensity of the image; a contraction of the polymer would be detected as a darkening of the image, whereas expansion would appear as image brightening. To evaluate the intercellular polymer matrix in biofilms, 3-day-old biofilms were exposed to similar solutions, and the resultant change in biofilm thickness was measured with LSM, which measures film thicknesses between 10 and 1,000 microns. The initial adhesive and biofilm polymers were similar in that both appeared to contract when treated with electrolytes and to expand when treated with Tween 20. However, with DMSO treatment, the initial adhesive polymer appeared to contract, whereas there was no change in thickness of the biofilm polymer. These results indicate that both polymers bear acidic groups and thus act electrostatically with cations and are able to enter into hydrophobic interactions.(ABSTRACT TRUNCATED AT 250 WORDS)

Adhesins, Bacterial↗

PubMed1994

Temperature-dependent absorption/desorption behavior of lower critical solution temperature (LCST) polymers on various substrates.

We have been studying adsorption and retention (resistance to desorption) behavior of temperature sensitive LCST polymers on different substrates as a function of temperature. According to our studies with Poly 64 (a copolymer of 60% (mol) NIPAAm and 40% (mol) NnBAAm, LCST = 8.5 degrees C in water), the copolymer retention depends on the rinse temperature. When the rinse temperature is above the LCST, the polymer adheres well to most surfaces. On the contrary, at rinse temperatures below the LCST, most of the adsorbed polymer is easily rinsed off. These studies are relevant to our work on the thermally reversible adsorption of LCST polymers conjugated to peptides and proteins, such as affinity ligands, for uses in immunoassays and affinity separations. The interaction between the LCST polymer and most hydrophobic polymer surfaces is mainly due to hydrophobic interactions, and the critical surface tension (gamma c) and the solubility parameter (delta) of the solid polymer substrate are the most important factors which influence the LCST polymer adsorption and retention. The critical surface tension appears to correlate best with the LCST polymer adsorption levels on different substrates, while the solubility parameter correlates best with the retention of the adsorbed polymer. According to our preliminary study, n-butyl groups probably interact more strongly with the substrates than isopropyl groups because of the greater hydrophobic surface area of the former groups.

Acrylamides↗

PubMed2004

Delayed intracranial delivery of a nitric oxide donor from a controlled-release polymer prevents experimental cerebral vasospasm in rabbits.

OBJECTIVE: Decreased local availability of nitric oxide (NO) may mediate chronic vasospasm after aneurysmal subarachnoid hemorrhage (SAH). Previous reports have shown that early treatment with NO prevents vasospasm in animals. We evaluated the efficacy of controlled-release polymers that contain the NO donor diethylenetriamine (DETA-NO) for the delayed treatment of vasospasm in a rabbit model of SAH. METHODS: DETA-NO 20% (wt/wt) was incorporated into ethylene-vinyl acetate (EVAc) polymers. Animals (n = 52) were randomized to two experimental groups. In the first group (n = 32), animals received SAH and implantation of either 20% DETA-NO/EVAc polymer at a dose of 0.5 mg/kg of DETA-NO (n = 16) or empty EVAc polymer (n = 16). Polymers were implanted 24 (n = 16) or 48 hours (n = 16) after SAH. In the second group (n = 20), animals received SAH and implantation of either 20% DETA-NO/EVAc polymer at a dose of 1.3 mg/kg (n = 10) or empty EVAc (n = 10). Polymers were implanted 24 (n = 10) or 48 hours (n = 10) after SAH. An additional group (n = 16) underwent either sham operation (n = 6) or SAH only (n = 10). Animals were killed 3 days after hemorrhage, and the basilar arteries were processed for morphometric measurements. Results were analyzed using Student's t test. RESULTS: Treatment with 20% DETA-NO/EVAc polymers at a dose of 1.3 mg/kg significantly increased basilar artery lumen patency when administered at 24 (97 +/- 6% versus 73 +/- 10%; P = 0.0396) or 48 hours (94 +/- 6% versus 71 +/- 9%; P = 0.03) after SAH. Treatment with 20% DETA-NO/EVAc polymers at a dose of 0.5 mg/kg administered 48 hours after SAH significantly increased lumen patency (82 +/- 8% versus 68 +/- 12%; P = 0.03); a dose of 0.5 mg/kg, 24 hours after SAH, did not reach statistical significance (74 +/- 7% versus 65 +/- 9%; P = 0.16). The SAH-only group had a lumen patency of 67 +/- 12%. CONCLUSION: Delayed treatment of SAH with controlled-release DETA-NO polymers prevented experimental posthemorrhagic vasospasm in the rabbit. This inhibition was dose-dependent. This further confirms the role of NO in the pathogenesis of vasospasm.

Animals↗

PubMed1999

Modification of the electrokinetic properties of reversible electrophoresis gels for the separation and preparation of DNA. Addition of linear polymers.

The effect of adding linear polymers to a novel reversible electrophoretic was measured. Reversible gels are formed using the polyanionic carbohydrate polymer, gellan gum. Gellan gum forms strong stable gels in the presence of divalent cations or diamines. The gels are reversible (return to solution) by changing the ionic environment or pH. Gellan gum is an anionic polymer, and the electrophoresis gels have considerable electroosmotic flow (EOF) toward the negative electrode. We measured the EOF in gellan gum electrophoresis gels as a function of gel concentration, buffer composition, and linear polymer additive. The linear polymers used in this study were polyethylene oxide and hydroxyethyl cellulose. Both polymers reduced EOF in the gels, in a manner dependent on molecular weight. Polymers with high molecular weight were more effective at reducing EOF. The addition of polymers increased the resolution of low molecular weight DNA. Native gellan gum resolved DNA from approx 50,000 to 1000 bp. Addition of the polymers resolved DNA down to approx 50 bp, in some instances. The influence of the polymers on circular plasmid DNA was also investigated. Addition of high molecular weight polyethylene oxide reduced the electrophoretic mobility of the nicked circular form compared to the supercoiled form.

DNA↗

PubMedDate not supplied

Microencapsulation using poly (L-lactic acid) III: Effect of polymer molecular weight on the microcapsule properties.

Poly (L-lactic acid) microcapsules were prepared using an emulsification and organic solvent evaporation technique (w/o system) with phenobarbitone as a reference core. Three polymers of different molecular weight (61,300; 43,200, 2400), were used to prepare different core loaded microcapsules. Microcapsule size increased with increase in polymer molecular weight. Microcapsule size was also found to increase with increase in core loading with the two high molecular weight polymers, whilst the low molecular weight polymer tended to aggregate to form larger microcapsules than expected. The calculated microcapsule density was found to decrease with an increase in the polymer molecular weight and core loading. 'Encapsulation efficiency' was reduced with the decrease in initial theoretical core loading. However, the phenobarbitone content of the microcapsules was not affected by the difference in polymer molecular weight. Significant morphological differences were observed due to variations in the polymer molecular weight. The two high molecular weight polymers were found to produce non-uniform, porous microcapsules, whilst low molecular weight polymer formed a uniform non-porous surface when core loading was low. With increasing core loading, an increasing number of phenobarbitone crystals were observed on the surface and microcapsules became increasingly porous. This was more evident after release of the drug. Differential scanning calorimetry of the microcapsules showed thermal events for both the polymer and phenobarbitone.

Chemical Phenomena↗