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PubMed1993

Programmable drug delivery from an erodible association polymer system.

An erodible association polymer system based on blends of cellulose acetate phthalate (CAP) and Pluronic F127, a block copolymer of poly(ethylene oxide) and poly(propylene oxide), has been investigated for its applicability to rate-programmed drug delivery. The compatibility and thermal properties were characterized by DSC and FTIR. Results from the thermal analysis indicate that the blends are compatible above 50% CAP, as revealed by a single composition-dependent glass transition temperature (Tg). The existence of molecular association through intermolecular hydrogen bonding between the carboxylic acid and the ether oxygen groups is supported by the observation of an upward shift in the IR carbonyl stretching frequency at increasing Pluronic F127 concentrations. Using theophylline as a model drug, the in vitro polymer erosion and drug release characteristics of the present polymer system were evaluated at different buffer pH's on a rotating-disk apparatus. The results show that the rates of both polymer erosion and drug release increase with the Pluronic F127 concentration in the blend. Further, at pH 4, the polymer erosion is minimal and the theophylline release appears to be governed mainly by diffusion through the polymer matrix. In contrast, at pH 7.4, the theophylline release is controlled primarily by the polymer surface erosion. To demonstrate the unique approach to programmed drug release based on the concept of nonuniform initial drug distribution, pulsatile patterns of drug release have been achieved successfully from the present surface-erodible polymer system using a multilaminate sample design with alternating drug-loaded layers.(ABSTRACT TRUNCATED AT 250 WORDS)

Biocompatible Materials↗

PubMed2003

The dawning era of polymer therapeutics.

As we enter the twenty-first century, research at the interface of polymer chemistry and the biomedical sciences has given rise to the first nano-sized (5-100 nm) polymer-based pharmaceuticals, the 'polymer therapeutics'. Polymer therapeutics include rationally designed macromolecular drugs, polymer-drug and polymer-protein conjugates, polymeric micelles containing covalently bound drug, and polyplexes for DNA delivery. The successful clinical application of polymer-protein conjugates, and promising clinical results arising from trials with polymer-anticancer-drug conjugates, bode well for the future design and development of the ever more sophisticated bio-nanotechnologies that are needed to realize the full potential of the post-genomic age.

Antineoplastic Agents↗

PubMed2001

Denture base polymer Alldent Sinomer: mechanical properties, water sorption and release of residual compounds.

The aim of this study was to determine flexural properties, water sorption, solubility and release of residual compounds of a new paste type denture base polymer Alldent Sinomer. In addition, an effort was made to reinforce the denture base polymer with a polymer-pre-impregnated glass fibre reinforcement (Stick). Six rhombic test specimens were fabricated for the flexural test in accordance to the ISO 1567 standard. Water sorption and solubility was also determined as described in the ISO standard. Residual compound release into water was determined with the high performance liquid chromatography (HPLC) METHOD: The flexural strength of Sinomer polymer was 85.8 MPa and flexural modulus 2.73 GPa. Storing of test specimens in water reduced the flexural strength and the modulus. By adding the glass fibre reinforcement into the test specimen, the flexural strength and the modulus increased considerably (ANOVA, P < 0.001). The increase was minor with the reinforcement of low fibre content and high with the reinforcement of higher fibre content. Water sorption of the Sinomer polymer was 26.4 microgram mm-3 and solubility was 1.52 microgram mm-3. High performance liquid chromatography analysis revealed the release of 0.18 wt% fraction of compound which was determined as methylmethacrylate (MMA) monomer. The results of this study suggest that the new denture base polymer Sinomer passed the requirements of the ISO standards and that its mechanical properties can be increased considerably by an incorporation of a glass fibre reinforcement. The release of MMA monomer into water from the polymer should be taken into account when the polymer is used in denture bases of patients with an allergy towards MMA.

Absorption↗

PubMed2004

Structure, surface excess and effective interactions in polymer nanocomposite melts and concentrated solutions.

The Polymer Reference Interaction Site Model (PRISM) theory is employed to investigate structure, effective forces, and thermodynamics in dense polymer-particle mixtures in the one and two particle limit. The influence of particle size, degree of polymerization, and polymer reduced density is established. In the athermal limit, the surface excess is negative implying an entropic dewetting interface. Polymer induced depletion interactions are quantified via the particle-particle pair correlation function and potential of mean force. A transition from (nearly) monotonic decaying, attractive depletion interactions to much stronger repulsive-attractive oscillatory depletion forces occurs at roughly the semidilute-concentrated solution boundary. Under melt conditions, the depletion force is extremely large and attractive at contact, but is proceeded by a high repulsive barrier. For particle diameters larger than roughly five monomer diameters, division of the force by the particle radius results in a nearly universal collapse of the depletion force for all interparticle separations. Molecular dynamics simulations have been employed to determine the depletion force for nanoparticles of a diameter five times the monomer size over a wide range of polymer densities spanning the semidilute, concentrated, and melt regimes. PRISM calculations based on the spatially nonlocal hypernetted chain closure for particle-particle direct correlations capture all the rich features found in the simulations, with quantitative errors for the amplitude of the depletion forces at the level of a factor of 2 or less. The consequences of monomer-particle attractions are briefly explored. Modification of the polymer-particle pair correlations is relatively small, but much larger effects are found for the surface excess including an energetic driven transition to a wetting polymer-particle interface. The particle-particle potential of mean force exhibits multiple qualitatively different behaviors (contact aggregation, steric stabilization, local bridging attraction) depending on the strength and spatial range of the polymer-particle attraction.

Computer Simulation↗

PubMed1997

Localization, depuration, bioaccumulation and impairment of ion regulation associated with cationic polymer exposure in rainbow trout (Oncorhynchus mykiss).

1. Static exposure of rainbow trout, Oncorhynchus mykiss, to three commercial 14C-labelled cationic polymers (EDP, epichlorhydrin-dimethylamine; CYT, polyacrylamide ester; and STK, polyacrylamide amide) resulted in 14C being concentrated only in gill tissue. 2. Depuration studies examining the effect of humic acid (HA) on cationic polymer bound in gill tissue indicate that the binding is reversible with exposure to polymer-free water and polymer-free water with HA for each of the three polymers. 3. Analysis of blood pH, Na+, K+, total NH3 and Cl- after static water exposures to EDP (m.w. 50,000) at 7.5 mg EDP/l revealed a treatment related decrease in blood pH, from 7.1 to 6.6, accompanied by an increase in blood NH3 and evidence of severe impairment of ion regulation. 4. Repeated exposure to the cationic polymers did not result in increases in the 14C concentration in gill tissue suggesting that bioaccumulation of the polymers does not occur. 5. These data suggest that the gill is the site of toxicity for these cationic polymers and that their toxic effects involve gill function and ion regulation rather than systemic actions on internal organs.

Acrylic Resins↗

PubMed2000

Evaluation of high molecular weight poly(oxyethylene) (Polyox) polymer: studies of flow properties and release rates of furosemide and captopril from controlled-release hard gelatin capsules.

The powder characteristics and the effect of the molecular weight of polymers as diluents on the release rate of furosemide and captopril from hard gelatin capsules were evaluated. The high molecular weight polymers studied were poly(oxyethylene) homopolymers (Polyox), with molecular weight ranging from 4,000,000 to 7,000,000. Powder characteristics suggested good flowability for these materials and predicted capsule fill weight uniformity. Swelling experiments showed a very high degree of swelling for these materials in both gastric and buffer solution. These polymers can sustain the release rate of both water-soluble and insoluble drugs from drug delivery systems. The low molecular weight polymers have a less pronounced sustained-release effect compared to the high molecular weight polymer material (i.e., those with 7,000,000 molecular weight). An increase in the content of polymer results in a decrease in the release rate of the drug. The solubility of the drugs clearly influenced the release rate. Release kinetics were evaluated and appeared to be influenced by the molecular weight of the polymer, the solubility of drug, and the ratio of the drug to polymer in the capsule. Bimodal release kinetics were exhibited by a number of furosemide formulations (i.e., F5 and F8).

Capsules↗

PubMed2005

In vitro release of levonorgestrel from phase sensitive and thermosensitive smart polymer delivery systems.

The objective of this research is to develop injectable controlled delivery systems for the contraceptive hormone, levonorgestrel (LNG), using phase sensitive and thermosensitive polymers. A combination of poly (lactide) (PLA) and a solvent mixture of benzyl benzoate (BB) and benzyl alcohol (BA) was used in the phase-sensitive polymer delivery systems. The effects of solvent systems and polymer concentrations on the in vitro LNG release were evaluated. In the case of thermosensitive polymer delivery systems, a series of low-molecular-weight poly (lactide-co-glycolide)-poly (ethylene glycol)-poly (lactide-co-glycolide) (PLGA-PEG-PLGA) triblock copolymers with varying ratios of lactide/glycolide (LA/GA, 2.0-3.5) were used. The effects of varying block length of copolymers 1, 2, 3, and 4 on the in vitro LNG release were evaluated. Phosphate buffer saline (pH 7.4) containing 0.5% w/v Tween-80 was used as in vitro release medium. The amount of the released LNG was determined by an high pressure liquid chromatography (HPLC) method. A controlled (zero-order) in vitro release of LNG was observed from both phase-sensitive and thermosensitive-polymer delivery systems. Increasing the concentration of the phase-sensitive polymer from 5% to 30% significantly (p < 0.05) decreased the release rate of LNG from 38.32 microg/day to 31.45 microg/day; and increasing the hydrophilic fraction of the solvents mixture (i.e., BA) significantly (p < 0.05) increased the release rate of LNG. In the case of the thermosensitive polymer delivery system, increasing the hydrophobic PLGA block length of copolymers significantly (p < 0.05) decreased the release rate of LNG (98.65 microg/day to 67.60 microg/day). It is evident from this study that both the phase sensitive and thermosensitive polymers are suitable for developing prolonged-release injectable delivery systems for the contraceptive hormone.

Benzoates↗

PubMed1996

Endovascular treatment of experimental aneurysms with liquid polymers: the protective potential of stents.

Liquid polymers have previously been used to treat experimental and human aneurysms. However, the delivery of a liquid embolic material into the cerebral circulation involves a high risk of irreversible vessel occlusion and stroke. To evaluate methods for the safe and effective treatment of experimental aneurysms with liquid polymer injection, we tested four different techniques to deliver cellulose acetate polymer (CAP) or N-hexyl-cyanoacrylate into canine side-wall carotid artery aneurysms. The animals were observed for 1 to 10 weeks after treatment. Two aneurysms were treated without protection of the distal circulation, one with CAP and another with N-hexyl-cyanoacrylate. In four cases, an angioplasty balloon was inflated within the parent artery during endosaccular injection of CAP. In two of these cases, the balloon was placed adjacent to the aneurysm orifice, resulting in simultaneous occlusion of both the aneurysm and the parent artery, and in the other two cases, the balloon was positioned proximal to the aneurysm, resulting in temporary flow arrest. Three aneurysms were treated with either CAP or N-hexyl-cyanoacrylate after implantation of a balloon-expandable tantalum stent within the parent artery across the aneurysm orifice. Complete angiographic obliteration was achieved in all but one case. One aneurysm ruptured. Another partially occluded aneurysm reopened 10 weeks after treatment. In all cases treated without stents, distal migration of the polymer resulted in either stenosis or occlusion of the parent arteries. The combination of stent implantation and polymer injection resulted in permanent aneurysm occlusion without detectable polymer migration. An intravascular stent deployed within the parent artery across the aneurysm orifice acted as a safety net during endosaccular polymer injection by allowing blood to flow from the aneurysm cavity while preventing distal migration of liquid polymer.

Aneurysm↗

PubMed1996

Biocompatible osteoconductive polymer versus iliac graft. A prospective comparative study for the evaluation of fusion pattern after anterior cervical discectomy.

STUDY DESIGN: One hundred fifteen patients having symptomatic cervical disc disease were recruited prospectively for this study. They were allocated randomly for either autologous iliac bone graft or biocompatible osteoconductive polymer implants. Both groups were compared clinically and radiologically. OBJECTIVES: Complications, long-term clinical and radiologic outcome, and hospital stay were compared to determine if biocompatible osteoconductive polymer was an improvement on iliac bone graft in terms of reduced donor site pain and shortened hospital stay. SUMMARY OF BACKGROUND DATA: Donor site morbidity is a significant problem in anterior cervical fusion. Hospital stay is another factor in the recent era of cost consciousness. Biocompatible osteoconductive polymer has been used in many centers as a biodegradable implant to circumvent these problems. METHODS: Smith-Robinson technique was used in 74 patients, and Cloward technique was used in 41 patients. Sixty-five patients had biocompatible osteoconductive polymer implants, and 50 patients had iliac bone graft. Patients were followed-up routinely in the outpatient clinic where pain visual analogue scale and Odom's criteria were used for outcome evaluation. Plain radiography, computed tomography scan, and magnetic resonance imaging were used for radiologic evaluation. RESULTS: The mean hospital stay was 4.8 days for those with iliac bone graft and 4.7 days for those with biocompatible osteoconductive polymer. Clinical outcome was identical in both groups. The incidence of partial graft protrusion and postoperative intersegmental kyphosis was statistically higher with iliac bone graft (P = 0.018 and P = 0.02, respectively). "Sclerosis" started to form around biocompatible osteoconductive polymer like a "halo" at 2 months. It increased with time, and sometimes was associated with new osteophyte formation; however, there was no biocompatible osteoconductive polymer incorporation or biodegradation CONCLUSIONS: Biocompatible osteoconductive polymer acts as a good "spacer" that reduces graft collapse and intersegmental kyphosis. However, it did not show any radiologic evidence of biodegradation or incorporation during the follow-up period of 24 months.

Adult↗

PubMed2006

Passage times for unbiased polymer translocation through a narrow pore.

We study the translocation process of a polymer in the absence of external fields for various pore diameters b and membrane thickness L. The polymer performs Rouse and reptation dynamics. The mean translocation time (tau(t)) that the polymer needs to escape from a cell and the mean dwell time (tau(d)) that the polymer spends in the pore during the translocation process obey scaling relations in terms of the polymer length N, L, and b/R(g), where R(g) is the radius of gyration for the polymer. We explain these relations using simple arguments based on polymer dynamics and the equilibrium properties of polymers.

Biological Transport↗

PubMed1979

Biosynthesis of glycosylated glycerolphosphate polymers in Streptococcus sanguis.

Two types of glycosylated glycerolphosphates were synthesized when a particulate enzyme prepared from Streptococcus sanguis was incubated with [3H]-phosphatidylglycerol and uridine diphosphate-[14C]glucose in the presence of MgCl2. The first type was extractable with saline and contained no fatty acid. The second type was pellet bound and could be extracted with 0.1% sodium dodecyl sulfate. Both types of polymers were purified and partially characterized. The first type of polymer was fractionated into five polymers, peaks 2a, 2b, 2c, 3a, and 3b. All except peak 2a, which contained only [3H]glycerol, contained both [3H]glycerol and [14C]glucose. [3H]NaBH4 reduction of acid hydrolysates of the polymers revealed that all of the polymers contained glucose as the major sugar componenta nd xylose as the minor sugar component. The second type of polymer was fractionated into three polymers, P-1, P-2, and P-3. All contained [3H]-glycerol, [14C]glucose, and fatty acids. P-1 appeared to be pure, whereas P-2 and P-3 contained two polymers each, as judged from sodium dodecyl sulfate-polyacrylamide gel electrophoresis.

Glucose↗

PubMed1992

Mass isotopomer distribution analysis: a technique for measuring biosynthesis and turnover of polymers.

Mass isotopomer distribution analysis (MIDA) is a technique for measuring biosynthesis and turnover of polymers in vivo. A stable isotopically enriched precursor is administered, and the relative abundances of different mass isotopomers in the polymer of interest are measured by mass spectrometry (MS). By comparison of statistical distributions predicted from the binomial or multinomial expansion to the pattern of excess isotopomer frequencies observed in the polymer, the enrichment of the biosynthetic precursor subunits (p) for newly synthesized polymers is calculated. MIDA thereby provides a solution to the problem of determining the isotope content in the actual precursor molecules that entered a particular polymeric product (the "true" precursor). The fraction of polymer molecules in a mixture that were newly synthesized during an isotopic experiment (fractional synthesis) can then be calculated. We describe some mathematical characteristics of MIDA and point out certain advantageous features. For example, mathematical estimates of p remain valid even if there does not exist a single anatomic or functional precursor pool. The interpretation of decay curves of endogenously labeled polymers may be improved by the use of higher mass isotopomers, which better fulfill the assumption of flash labeling. By combining fractional synthesis values with rate constants of decay, absolute endogenous synthesis rates can be calculated. Thus, by using probability logic combined with MS analysis, MIDA allows dynamic measurements to be made through analyses on a polymer alone during both isotopic incorporation and decay phases. The method has been applied to fatty acids, cholesterol, and glucose and is potentially applicable to nucleic acids, porphyrins, perhaps proteins, and many other classes of polymers.

Indicator Dilution Techniques↗

PubMed2002

Vascular response to infusions of a nonextravasating hemoglobin polymer.

The clinical utility of cross-linked tetrameric hemoglobin solutions is limited by peripheral vasoconstriction thought to be due to scavenging of nitric oxide. In addition, transfusion of crude preparations of hemoglobin polymers can cause arterial hypertension. We tested the hypothesis that eliminating low-molecular-weight components from the polymer solution would prevent extravasation and its associated pressor response. A zero-link polymer of bovine hemoglobin was developed without chemical linkers left between the tetramers. Transfusion of unprocessed preparations of these polymers in rats resulted in appearance of the polymer in the renal hilar lymph. However, eliminating the low-molecular-weight components with a 300-kDa diafiltration resulted in an average hydrodynamic radius of 250 A and in undetectable levels of polymer in hilar lymph. Exchange transfusion in anesthetized rats and cats and in awake cats produced no increase in arterial pressure. In anesthetized cats, exchange transfusion with an albumin solution reduced hematocrit from 30 to 18%, increased cerebral blood flow, and dilated pial arterioles. In contrast, reducing hematocrit by transfusing the diafiltered polymer did not increase cerebral blood flow as pial arterioles constricted. These results are consistent with the hypothesis that the increase in arterial pressure associated with cell-free hemoglobin transfusion depends on hemoglobin extravasation. Constriction observed in the cerebrovascular bed with a nonextravasating hemoglobin polymer at low hematocrit is presumably a regulatory response to prevent overoxygenation at low blood viscosity.

Animals↗

PubMed2002

Importance of a biofouling-resistant phospholipid polymer to create a heparinized blood-compatible surface.

Heparinization is believed to be one of the methods to suppress thrombus formation on blood-contacting surfaces. However, this study hypothesizes that heparinization alone might not be sufficient to provide a blood-compatible surface; that is, a surface property that resists biofouling is necessary to obtain an effective heparin-modified surface. 2-Methacryloyloxyethyl phosphorylcholine (MPC) polymers with 2-aminoethyl methacrylate (AEMA) were synthesized to immobilize heparin through ionic bonding. The primary amino groups of AEMA were considered to be the polymer surface because the zeta-potential of the surface was positive when the mole fraction of the AEMA units was above 0.2. The antithrombogenic character of the polymer surface modified with heparin was evaluated by both Lee-White and microsphere column methods. The coagulation period of human whole blood in the absence of anticoagulant in glass tubing coated with the MPC polymer was longer than that in the original glass tube. Cell adhesion was completely inhibited on the MPC polymer surface after contact with human whole blood without anticoagulant. However, many adherent blood cells were observed on poly(2-ethylhexyl methacrylate-co-AEMA) (no MPC unit) even after heparinization. These results strongly indicate that the MPC polymer is a useful substrate where the heparin works well and that the heparin-immobilized MPC polymer has superior blood compatibility to the simple MPC polymer.

Anticoagulants↗

PubMed1990

Protein adsorption on polymer surfaces: calculation of adsorption energies.

In an attempt to understand the mechanisms of protein adsorption at the solid-liquid interface, we have calculated the interaction potential energy between the protein and the polymer surface by a computer simulation approach. The adsorption of four proteins--lysozyme, trypsin, immunoglobulin Fab, and hemoglobin--on five polymer surfaces was examined. The model polymers used for the calculation were polystyrene, polyethylene, polypropylene, poly(hydroxyethyl methacrylate), and poly(vinyl alcohol). All possible orientations of the protein on the polymer surfaces were simulated and the corresponding interaction energies for the initial contact stage of protein adsorption were calculated. In the calculation of interaction energies, the hydrophobic interaction was not treated explicitly owing to the difficulty in the theoretical treatment. The results showed that the interaction energy was dependent on the orientation of the protein on the polymer surfaces. The energy varied from -850 to +600 kJ/mol with an average of about -155 kJ/mol. The interaction energy was also dependent on the type of polymer. The average interaction energies of the four proteins with poly(vinyl alcohol) were always lower than those with the other polymers. The interaction energy was not dependent on the protein size. It was found that the dispersion attraction played the major role in protein adsorption on neutral polymer surfaces.

Adsorption↗

PubMed1994

The chemiluminescence response of neutrophils on polymer surfaces made by glow discharge plasma polymerization.

Polypropylene tubes were coated with different polymers made by glow discharge plasma polymerization. Isolated human blood neutrophils were allowed to interact with the polymer surface and the chemiluminescence response of the cells was recorded as a measure of oxidative activation. The polymers represented surfaces that differed markedly with respect to charge, hardness, and wettability. We found that all polymers stimulated the chemiluminescence response in neutrophils differently; when preincubation with human serum albumin (HSA) there was a general reduction of the chemiluminescence response particularly on one of the positively charged surface 1,2-diamino-cyclohexane (DACH). Addition of a soluble stimulus, the chemoattractant formylmethionyl-leucylphenylalanine (FMLP), to the cells caused a dramatic increase in the response on one of the hydrophobic surface hexamethylene-disiloxane (HMDSO). However, there was also a pronounced reduction in the response on polymers with acrylic acid (AA). The response was normalized after addition of HSA. Taken together, the chemiluminescence response of the neutrophils interacting with the polymer surfaces differed with regard to the type of surfaces. When HSA and FMLP were added a larger difference in the response was found. Our results showed that the activation of human neutrophil granulocytes influenced by different polymer surfaces, followed unspecific different patterns which were someway related to the specific characteristics of the polymer and from this point we came to similar conclusions made by Kaplan et al. (J. Biomater. Res. 28, 377 (1994)), that it is difficult to extrapolate any activation mechanisms from one material to another.(ABSTRACT TRUNCATED AT 250 WORDS)

Acrylates↗

PubMed1994

Fusogenic activity of various water-soluble polymers.

The fusogenic activity of seven water-soluble polymers was investigated using L929 cells in a monolayer state. Among these polymers, only two, poly(ethylene glycol) (PEG) and EPAN 680 were capable of inducing the membrane fusion of L929 cells. EPAN 680 is an ABA type block copolymer composed of 80% ethylene oxide(A) and 20% propylene oxide(B) sequences with a total molecular weight of 8800. Evaluation of the polymer hydrophobicity indicated that there was no clear correlation between it and the fusogenic activity of the polymer, although highly hydrophobic polymers caused cell shrinkage without membrane fusion. Differential scanning calorimetry on these polymers strongly suggested that hydration of the polymers in culture medium had a large effect on their fusogenic activity. It was concluded that the assembly of cell membranes, stabilized by water molecules, was disturbed by strong interaction with the polymer molecules having a strong hydration power, resulting in membrane fusion.

Animals↗

PubMed1987

Rapid formation of large molecular weight alpha-polymers in cross-linked fibrin induced by high factor XIII concentrations. Role of platelet factor XIII.

After fibrin polymerization, activated Factor XIII catalyzes the formation of intermolecular cross-links between gamma-chain pairs and also among two or more alpha-chains to form polymers. In this report we characterize the size and heterogeneity of alpha-chain polymers, establish the role of high concentrations of Factor XIII in determining the extent and rate of alpha-polymer formation, and also provide evidence that the Factor XIII required can be provided by platelets. Fibrin prepared from purified fibrinogen or platelet-deficient plasma contained a series of cross-linked alpha-chain polymers with Mr from 140,000 to 770,000 with a mean Mr difference of 32,000 consistent with a staggered, overlapping addition of monomers to the growing alpha-polymer chain. In plasma containing no platelets, alpha-polymer formation was incomplete with residual alpha-monomer remaining, but higher platelet counts facilitated more rapid cross-linking into larger polymers. Purified Factor XIII was equally effective as platelets in facilitating cross-linking. We conclude that cross-linked alpha-polymer chains are heterogeneous in size reaching a molecular weight of several million and that high concentrations of Factor XIII as provided by platelets are required for maximum cross-linking.

Blood Platelets↗