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PubMed2003

In vitro biocompatibility assessment of sulfonated polyrotaxane-immobilized polyurethane surfaces.

Sulfonated polyrotaxanes (PRx-SO(3)'s), in which sulfonated alpha-cyclodextrins (alpha-CDs) were threaded onto the poly(ethylene glycol) (PEG) segments in a PEG-b-poly(propylene glycol) (PPG)-b-PEG triblock copolymer (Pluronic) capped with benzyloxycarbonyl (Z)-L-phenylalanine (Z-L-Phe), were prepared as a novel surface-modifying biomaterial. Surface modification of the polyurethane (PU) was carried out by blending the PRx-SO(3)'s with a PU solution, followed by solution casting. The incorporated PRx-SO(3)'s led to the enhanced hydrophilicity by changing the surface properties of the PU matrix. Modified PUs showed the stable entrapment of the PRx-SO(3)'s with little extraction into water and enhanced mechanical properties after exposure to water compared to the PU control. The incorporated PRx-SO(3)'s repelled the proteins and kept them from closely approaching the surface areas, prevented platelet activation by thrombin, and effectively repelled bacteria. These results suggest that both the supramolecular structure of the polyrotaxanes and exposure of the sulfonated groups onto the surfaces contribute to these phenomena. Thus, surface modification with PRx-SO(3)'s is suggested to be useful for the fabrication of biocompatible medical devices.

Biocompatible Materials↗

PubMed2004

Peripheral blood cell separation through surface-modified polyurethane membranes.

Cell separation from peripheral blood was investigated using surface-modified polyurethane (PU) membranes with different functional groups. Both red blood cells and platelets could pass through unmodified PU and PU-SO(3)H membranes, whereas the red blood cells preferentially passed through PU-N(C(2)H(5))(2) and PU-NHC(2)H(4)OH membranes. The permeation ratio of T and B cells was <25% for the surface-modified and unmodified PU membranes. CD34(+) cells have been recognized as various kinds of stem cells including hematopoietic and mesenchymal stem cells. The adhesiveness of CD34(+) cells on the PU membranes was found to be higher than that of red blood cells, platelets, T cells, or B cells. Overall, the adhesiveness of blood cells on the PU membranes increased in the following order: red blood cells </= platelets < T cells </= B cells < CD34(+) cells. Treatment of PU-COOH membranes with a human albumin solution to detach adhered blood cells, allowed recovery of mainly CD34(+) cells in the permeate, whereas both red blood cells and platelets could be isolated in the permeate using unmodified PU membranes. The PU membranes showed different permeation and recovery ratios of specific cells depending on the functional groups attached to the membranes.

Antigens, CD↗

PubMed2003

Engineering porous polyurethane scaffolds by photografting polymerization of methacrylic acid for improved endothelial cell compatibility.

Using a preadsorbing-monomer method, polyurethane (PU) porous scaffolds were modified by grafting polymerization of methacrylic acid (MAA) initiated under UV light. Fourier transform infrared-attenuated total reflection spectroscopy and X-ray photoelectron spectroscopy characterizations confirmed the occurrence of the grafting polymerization of poly(methacrylic acid) (PMAA) on PU scaffolds and the measurement of water adsorption also demonstrated enhanced hydrophilicity. The PMAA grafting degree correlated to the amount of MAA adsorbed, the pore average diameter, and the porosity. It was verified that the higher porosity the scaffold has, the larger porous area (or the larger contact area with MAA) it has, and therefore the higher amount of MAA adsorbed and higher grafting degree obtained. The results of human endothelial cells cultured in vitro showed that the PU scaffolds modified with the hydrophilic PMAA had more improved cell compatibility than the control matrix.

Cell Adhesion↗

PubMed2004

Gene expression changes in BALB/3T3 transformants induced by poly(L-lactic acid) or polyurethane films.

We performed DNA microarray analysis on two BALB/3T3 transformants (A5 and A6) induced by polyurethane (PU) film, two (L11 and L21) induced by biodegradable poly(L-lactic acid) (PLLA) film, and the parental cells. The transforming ability of the cells was in the order A5 < A6 < L21 < L11. In all, 1176 cancer-related genes were up- or down-regulated in at least one transformant. Those that were markedly up-regulated were c-fos protooncogene, FBJ osteosarcoma oncogene B, and Jun oncogene; those markedly down-regulated were pleiotrophin, histidine triad nucleotide-binding protein, protein kinase C iota, and large multifunctional protease 7. A common function of proteins encoded by genes that underwent marked expression changes was bone formation. The genes were c-fos, FBJ osteosarcoma, Jun, pleiotrophin, a disintegrin-like and metalloprotease with TS-1 motif protein 1. This finding was consistent with the tumor formation in the 2-year PLLA or PU subcutaneous implantation into rats. The number of genes that underwent marked expression change in each transformant was consistent with its malignancy. PLLA induced more malignant transformants than PU, especially in relation to osteosarcoma-like gene expression.

Animals↗

PubMed2004

Effect of soft-segment chemistry on polyurethane biostability during in vitro fatigue loading.

The effect of soft-segment chemistry on biostability of polyurethane elastomers was studied with a diaphragm-type film specimen under conditions of static and dynamic loading. During testing, the films were exposed to an H(2)O(2)/CoCl(2) solution, which simulated the oxidative component of the in vivo environment. Films treated for up to 24 days were evaluated by IR spectroscopy and by optical and scanning electron microscopy. Biostability of a poly(ether urethane) (PEU), which is known to undergo oxidative degradation, was compared with biostability of a poly(carbonate urethane) (PCU), which is thought to be more resistant to oxidation than PEU. Materials similar to PEU and PCU, in which the polyether or polycarbonate soft segment was partially replaced with poly(dimethylsiloxane) (PDMS), were also tested with the expectation that PDMS would improve soft-segment biostability. Oxidative degradation of the polyether soft segment of PEU was manifest chemically as chain scission and cross-linking and physically as surface pitting. Biaxial fatigue accelerated chemical degradation of PEU and eventually caused brittle stress cracking. In comparison, the polycarbonate soft segment was more stable to oxidation; there was minimal chemical or physical degradation of PCU, even in biaxial fatigue. Partial substitution of the polyether soft segment with PDMS enhanced oxidative stability of PEU. Although both strategies for modifying soft-segment chemistry improved the resistance to oxidative degradation, the outstanding mechanical properties of PEU were compromised to some extent.

Biocompatible Materials↗

PubMed2004

Cell separation of hepatocytes and fibroblasts through surface-modified polyurethane membranes.

The separation of fibroblast cells (L929 cells) and hepatocytes was investigated by using unmodified and surface-modified polyurethane (PU) foaming membranes (pore size of 12 microm) by the incorporation of various functional groups. L929 cells permeated more readily than hepatocytes, and very few populations of hepatocytes (<5%) permeated through the membranes. This result was thought to be due to the smaller cell size of the L929 cells (5-10 microm) relative to the hepatocytes (15-30 microm). The larger hepatocytes were thought to plug the pores of the membranes. A good cell separation between L929 cells and hepatocytes was achieved when the cell mixture permeated through the negatively charged PU membranes. The negatively charged membranes were thought to enhance the permeation of L929 cells because of the electrostatic repulsion between the membranes and negatively charged cells. On the other hand, the hepatocytes were unable to permeate through the membranes because of the sieve effect caused by their large cell size. The separation of hepatocytes isolated from mice at different ages was also accomplished by permeating the cell mixture through unmodified and surface-modified PU membranes.

Animals↗

PubMed2005

In vitro interaction of human fibroblasts and platelets with a shape-memory polyurethane.

Physicochemical and mechanical properties, in vitro cytotoxicity, cytocompatibility, and platelet adhesion were investigated on a shape-memory polyether-based polyurethane (MM-5520 SMPu) using the polyether-based Pellethane 2363-80AE (Pell-2363 SPU) as reference. MM-5520 SMPu and Pell-2363 SPU showed similar average molecular weights and different surface properties, with a higher hydrophilicity and roughness for the SMPu. By tensile tests and dynamic mechanical analysis, the peculiar characteristics of the MM-5520 SMPu were evidenced: strong temperature-dependent behavior for SMPu compared with SPU, and a high shape recovery. MM-5520 SMPu did not show any cytotoxic effect on the adhesion and proliferation of human skin fibroblasts and gingival fibroblasts, and a good cytocompatibility was observed with both cell types, as demonstrated by cell counting and scanning electron microscopy observations. SMPu compared with SPU showed higher adsorption of extracellular matrix proteins such as fibronectin, fibrinogen, and collagens. Proteins adsorbed onto SMPu significantly enhanced the adhesion and proliferation of human fibroblasts. The interaction of SMPu with platelets was studied with platelet rich plasma. Fewer platelets adhered to the SMPu, with minor morphological variations than onto the SPU. The cytocompatibility and hemocompatibility of MM-5520 SMPu combined with its unique properties such as change in shape or in stiffness, depending on practical requirements, make this shape-memory material potentially advantageous for biomedical applications.

Adsorption↗

PubMed2005

Mechano-active scaffold design of small-diameter artificial graft made of electrospun segmented polyurethane fabrics.

To fabricate a "mechano-active" tubular scaffold of nonwoven mesh-type small-diameter artificial graft made of the synthetic durable elastomer, segmented polyurethane, the fabrication technique of electrospinning on a mandrel under a high rotation speed and transverse movement was used. Emphasis was placed on how the rotation speed of the mandrel and the fusion or welding states of fibers at contact points affect the compliance (ease of intraluminal pressure-dependent circumferential inflation) and Young's modulus determined by uniaxial stretching in the longitudinal and circumferential directions. The results showed that a high rotation speed is attributed to exhibit isotropic mechanical properties in the entire range of applied strain but reduces the compliance, and a high fusion state, which is produced using a mixed solvent with a high content of high-boiling-point solvent, reduces the compliance but is expected to exhibit high durability in a continuously loaded pulsatile stress field in an arterial circulatory system.

Artificial Organs↗

PubMed2005

Role of protein kinase C in the monocyte-derived macrophage-mediated biodegradation of polycarbonate-based polyurethanes.

Polycarbonate-polyurethanes (PCNUs) elicit a foreign body reaction during the initial tissue contact, partly mediated by the respiratory burst in monocytes, during which protein kinase C (PKC) activates NADPH (nicotinamide adenine dinucleotide phosphate) oxidase. Using an in vitro cell system, monocytes were differentiated into monocyte-derived macrophages (MDMs) and then reseeded onto three PCNUs (HDI431, HDI321, or MDI321): hexane (HDI) or 4,4-methylene bis-phenyl (MDI) diisocyanates synthesized with poly(1,6-hexyl 1,2-ethyl carbonate) diol (PCN) and 14C-labeled butanediol (BD) in the ratios 4:3:1 or 3:2:1 (diisocyanate/PCN/BD). MDM-mediated degradation was assessed by radiolabel release in the presence of a PKC activator (phorbol myristate acetate), inhibitor (H7), and a catalase/peroxidase inhibitor (NaN3). Activating PKC decreased biodegradation and esterase activity in MDMs on HDI431 and HDI321 but not MDI321, whereas H7 and NaN3 inhibited the MDM degradation of MDI321 only. Pretreatment of the PCNUs with H2O2 inhibited esterase-mediated radiolabel release from HDI431 and HDI321 but stimulated radiolabel release from MDI321. The difference in the effect of H2O2 on the HDI versus MDI PCNUs contributes to explaining the effect of PKC activation on material degradation. Understanding the mechanism by which this pathway is linked to PCNU chemistry may assist in designing materials with tailored biodegradation rates.

1-(5-Isoquinolinesulfonyl)-2-Methylpiperazine↗

PubMed2005

The role of adsorbed fibrinogen in platelet adhesion to polyurethane surfaces: a comparison of surface hydrophobicity, protein adsorption, monoclonal antibody binding, and platelet adhesion.

Ten specially synthesized polyurethanes (PUs) were used to investigate the effects of surface properties on platelet adhesion. Surface composition and hydrophilicity, fibrinogen (Fg) and von Willebrand's factor (vWf) adsorption, monoclonal anti-Fg binding, and platelet adhesion were measured. PUs preadsorbed with afibrinogenemic plasma or serum exhibited very low platelet adhesion, while adhesion after preadsorption with vWf deficient plasma was not reduced, showing that Fg is the key plasma protein mediating platelet adhesion under static conditions. Platelet adhesion to the ten PUs after plasma preadsorption varied greatly, but was only partially consistent with Fg adsorption. Thus, while very hydrophilic PU copolymers containing PEG that had ultralow Fg adsorption also had very low platelet adhesion, some of the more hydrophobic PUs had relatively high Fg adsorption but still exhibited lower platelet adhesion. To examine why some PUs with high Fg adsorption had lower platelet adhesion, three monoclonal antibodies (mAbs) that bind to sites in Fg thought to mediate platelet adhesion were used. The antibodies were: M1, specific to gamma-chain C-terminal; and R1 and R2, specific to RGD containing regions in the alpha-chain N- and C-terminal, respectively. Platelet adhesion was well correlated with M1 binding, but not with R1 or R2 binding. When these mAbs were incubated with plasma preadsorbed surfaces, they blocked adhesion to variable degrees. The ability of the R1 and R2 mAbs to partially block adhesion to adsorbed Fg suggests that RGD sites in the alpha chain may also be involved in mediating platelet adhesion and act synergistically with the C-terminal of the gamma-chain.

Adsorption↗

PubMed2005

In vivo biostability of polyether polyurethanes with polyethylene oxide surface-modifying end groups; resistance to biologic oxidation and stress cracking.

Polyethylene oxide (PEO) on polymer surfaces has been reported to reduce cellular adhesion, a very desirable property for cardiac pacing leads. A Shore 80A polyether polyurethane with up to 6% PEO surface-modifying end groups (SME) was evaluated for its chronic in vivo biostability. In a short-term (12 week) screening test, strained samples appeared to develop the same surface oxidation as unmodified polymer, but did not produce visible cracking > or =500x, prompting a longer-term study. By the time the longer-term study was initiated, most of the PEO SME had disappeared from the starting material's surface. After 1 year in vivo, surface oxidation, shallow surface cracking, and environmental stress cracking (ESC) developed on highly strained samples to the point of failure, so that there was no significant difference between the SME polymer and its control (the same polymer without SME). No further change was seen for up to 2 years of implantation. Unstrained PEO SME polymer developed shallow surface cracking, but no ESC up to 2 years of implantation. Thus, PEO SME slightly delayed, but did not stop biodegradation, and under unstrained conditions, has no adverse effect on biostability.

Absorbable Implants↗

PubMed2005

Hydrolytic degradation behavior of biodegradable polyetheresteramide-based polyurethane copolymers.

In this article, a new kind of biodegradable polyetheresteramide-based polyurethane (PEEA-U) copolymers were prepared by the melt polycondensation method from epsilon-caprolactone, 6-aminocaproic acid, poly(ethylene glycol), and toluene diisocyanate. The water absorption of PEEA-U was affected strongly by the reaction time and the content of chain extender; and the hydrolytic degradation behavior of the copolymers was mainly determined by the reaction time, chain extender content, and the pH value of the degradation medium. Also, DSC, (1)H-NMR, and inherent viscosity were used to characterize the degradation behavior of the copolymers.

Absorbable Implants↗

PubMed2006

A long-term in vitro biocompatibility study of a biodegradable polyurethane and its degradation products.

The biological safety of degradation products from degradable biomaterials is very important. In this study a new method is proposed to test the cytotoxicity of these degradation products with the aim to save time, laboratory animals, and research funds. A biodegradable polyurethane (PU) foam was subjected to this test method. The PU had soft segments of DL-lactide/epsilon-caprolactone and hard segments synthesized from butanediol and 1,4-butanediiosocyanate. Copolymer foams without urethane segments, consisting of DL-lactide/epsilon-caprolactone, were tested as well. Accumulated degradation products were collected by degrading the foams in distilled water at 60 degrees C up to 52 weeks. Cell-culture medium was prepared from powder medium with this water. In different tests the cytotoxicity of this medium was established. The first signs of cytotoxicity were observed after 3-5 weeks of degradation. This accounts for both materials and reestablishes the good short-term biocompatibility of these materials. The PU showed more toxicity toward the end stages of degradation in comparison with the copolymer. This is probably related to the accumulation of degradation products of the urethane segments. In the in vivo situation the degradation of the PU and the metabolism and excretion of degradation products may differ. Therefore, long-term in vivo studies will have to establish whether these in vitro results are representative for the in vivo behavior of the degrading PU.

Absorbable Implants↗

PubMed2006

Fabrication of microporous polyurethane by spray phase inversion method as small diameter vascular grafts material.

Microporous polyurethane vascular prostheses with a 4 mm diameter and 0.3-0.4 mm wall thickness were fabricated by a spray phase inversion technique. In this study, the effect of distance between spray guns (SG) and rotating mandrel (RM), the effect of rate of rotating mandrel (RRM), and the type of nonsolvent on pore morphology of PU films were evaluated using scanning electron microscopy (SEM) technique. It was observed that when the distance between SG and RM was increased or the rate of RM was decreased, the porosity of PU films increased and consequently the tensile strength decreased and compliance value increased. Compliance was measured in vitro by volume and vessel diameter changes. Furthermore, when the coagulant (water) was changed to the water/methanol, the porosity of PU film increased and porous morphology changed to filamentous morphology. Attachment of anchorage dependent cells, namely L929 fibroblast cells, were investigated in stationary culture conditions. The cells adhesion and cells growth were studied using optical photomicrographs. The results show that by increasing the porosity content of PU films would consequently increase the cell ingrowths.

Animals↗

PubMed2006

Separation of CD34+ cells from human peripheral blood through polyurethane foaming membranes.

Cell separation from peripheral blood was investigated using polyurethane (PU) foaming membranes and PU membranes (pore size, 5 or 12 mum) at different blood permeation speeds. Permeation ratio of hematopoietic stem cells (CD34(+) cells) through the PU membranes was the lowest among the blood cells at any blood permeation speed. This is thought to be because CD34(+) cells are more adhesive than red blood cells (RBCs), platelets, T cells, and B cells. Primitive hematopoietic stem and progenitor cells tend to adhere to the surface of mature blood cells, because of the high expression of cell-adhesion molecules on the surface of the cells. Human serum albumin solution was exposed to PU-COOH membranes to detach adhered cells from the surface of the membranes, allowing isolation of CD34(+) cells and reduction of RBCs in the permeate solution. Most purified CD34(+) cells (high recovery ratio of CD34(+) cells divided by recovery ratio of RBCs) were obtained in the recovery process using PU-COOH membranes (pore size, 5.2 microm) at a permeation speed of 0.3-1 mL/min.

Adult↗

PubMed2006

Stress response of adherent cells on a polymer blend surface composed of a segmented polyurethane and MPC copolymers.

To better understand the effect of 2-methacryloyloxyethyl phosphorylcholine (MPC) copolymer in improving the biocompatibility of segmented polyurethane (SPU), the expression of heat shock protein (HSP) mRNA in HeLa S3 cells adhered on SPU blended with MPC copolymers was measured. Conventionally, MPC copolymers (PMEH) were synthesized by changing the feed ratios of MPC and 2-ethylhexyl methacrylate. X-ray photoelectron spectroscopic analysis of the SPU/PMEH film indicated that the surface concentration of MPC units on the SPU/PMEH film increased with an increase in PMEH composition. HeLa S3 cells were cultured on SPU/PMEH films. The number of adherent cells on the SPU/PMEH films decreased with an increase in the concentration of PMEH. When the PMEH composition was greater than 0.5 wt %, cell adhesion and proliferation decreased markedly. Expressions of HSP27 and HSP47 mRNA were detected using the reverse transcription-polymerase chain reaction (RT-PCR). After incubation for 24 h, both the HSP mRNA expressions in the HeLa S3 cells showed no significant differences among all samples. In HeLa S3 cells that adhered to the SPU film for 48 h, the expressions of HSP27 and HSP47 mRNA increased significantly when compared with those incubated for 24 h. In contrast, the two kinds of mRNA expressions decreased in the HeLa S3 cells that adhered to the SPU/PMEH films for 48 h. From these results, we concluded that PMEH was quite important in suppressing the stress response of adherent HeLa S3 cells. Therefore, SPU/PMEH blend polymers are useful as implantable biomedical materials.

Adsorption↗

PubMed2006

Prevention of oxidative degradation of polyurethane by covalent attachment of di-tert-butylphenol residues.

Polyurethane (PU) components of cardiovascular devices are subjected to oxidation-initiated surface degradation, which leads to cracking and ultimately device failure. In the present study, we investigated a novel bromoalkylation chemical strategy to covalently attach the antioxidant, di-tert-butylphenol (DBP), and/or cholesterol (Chol) to the PU urethane nitrogen groups to hypothetically prevent oxidative degradation. These experiments compared PU, PU-DBP, PU-Chol, and PU-Chol-DBP. A series of comparative oxidative degradation studies involved exposing PU samples (modified and unmodified) to H2O2-CoCl2 for 15 days at 37 degrees C, to cause accelerated oxidative degradation. The extent and effects of degradation were assessed by attenuated total reflectance Fourier transformation infrared spectroscopy (FTIR), scanning electron microscopy (SEM), surface contact angle measurements, and mechanical testing. Both the Chol and DBP modification conferred significant resistance to oxidation related changes compared to unmodified PU per FTIR and SEM results. SEM demonstrated cavitation only in unmodified PU. However, contact angle analysis showed significant oxidation-induced changes only in the Chol-modified PU formulations. Most importantly, uniaxial stress-strain testing revealed that only PU-DBP demonstrated bulk elastomeric properties that were minimally affected by oxidation; PU, PU-Chol, PU-Chol-DBP showed marked deterioration of their stress-strain properties following oxidation. In conclusion, these results demonstrate that derivatizing PU with DBP confers significant resistance to oxidative degradation compared with unmodified PU.

Butanes↗

PubMed2007

Protein adsorption on polyurethane catheters modified with a novel antithrombin-heparin covalent complex.

Highly anticoagulant covalent antithrombin-heparin complex (ATH) was covalently grafted onto polyurethane catheters to suppress adsorption/activation of procoagulant proteins and enhance adsorption/activation of anticoagulant proteins for blood compatibility. Consistency of catheter coating was demonstrated using immunohistochemical visualization of ATH. The ability of the resulting immobilized ATH heparin chains to bind antithrombin (AT) from plasma, as measured by binding of (125)I-radiolabeled AT, was greater than that for commercially-available heparin-coated catheters, and much greater than for uncoated catheters. Complementary measurements of antifactor Xa (FXa) activity and plasma protein binding were also performed. Both ATH-coated and heparin-coated catheters demonstrated functional binding of exogenous AT. However, the ATH-coated catheters gave a trend towards elevated anti- FXa activities/AT binding ratios, consistent with the higher active pentasaccharide content in starting ATH. Western blot analysis of proteins adsorbed to catheters after incubation with rabbit plasma established protein binding profiles that showed AT and albumin as major plasma proteins adsorbed to ATH-coated catheters, while AT and altered forms of fibrinogen were major plasma protein species adsorbed to heparinized catheters.

Adsorption↗