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1.
Langmuir ; 30(22): 6489-96, 2014 Jun 10.
Artigo em Inglês | MEDLINE | ID: mdl-24832682

RESUMO

In this work, the hemocompatibility of polyampholyte copolymers from the mixed-charge copolymerization of negatively charged 3-sulfopropyl methacrylate (SA) and positively charged [2-(methacryloyloxy)ethyl] trimethylammonium (TMA) was studied. Charge-bias variation of the prepared poly(SA-co-TMA) copolymers can be controlled using the regulated SA and TMA monomer ratio via homogeneous free radical copolymerization. A systematic study of how charge-bias variations in poly(SA-co-TMA) copolymers affect the hemocompatibility in human blood plasma was reported. The hydrodynamic size of prepared polymers and copolymers is determined to illustrate the correlations between intermolecular cationic/anionic associations and the blood compatibility of polySA, poly(SA-co-TMA), and polyTMA suspensions in human blood plasma. It was found that the protein resistance and hydration capability of prepared copolymers can be effectively controlled by regulating the charge balance of the SA/TMA compositions in poly(SA-co-TMA). The results suggest that polyampholyte copolymers of poly(SA-co-TMA) with overall charge neutrality have a high hydration capability and the best antifouling, anticoagulant, and antihemolytic activities as well as zwitterionic sulfobetaine-based homopolymers when in contact with blood plasma at human body temperature.


Assuntos
Materiais Biocompatíveis/química , Polímeros/química , Materiais Biocompatíveis/efeitos adversos , Humanos , Metacrilatos/química , Polímeros/efeitos adversos
2.
Biomacromolecules ; 13(9): 2849-58, 2012 Sep 10.
Artigo em Inglês | MEDLINE | ID: mdl-22838402

RESUMO

"Schizophrenic" diblock copolymers containing nonionic and zwitterionic blocks were prepared with well-controlled molecular weights via atom-transfer radical polymerization (ATRP). In this work, we report a systematic study of how morphological changes of poly(N-isopropylacrylamide)-block-poly(sulfobetaine methacrylate) (PNIPAAm-b-PSBMA) copolymers affect hemocompatibility in human blood solution. The "schizophrenic" behavior of PNIPAAm-b-PSBMA was observed by (1)H NMR, dynamic light scattering (DLS), and turbidity measurement with double morphological transition, exhibiting both lower critical solution temperature (LCST) and upper critical solution temperature (UCST) in aqueous solution. Below the UCST of PSBMA block, micelles were obtained with a core of insoluble PSBMA association and a shell of soluble PNIPAAm, whereas the opposite micelle structure was observed above the LCST of PNIPAAm block. In between the UCST and LCST, unimers with both soluble blocks were detected. Hydrodynamic size of prepared polymers and copolymers is determined to illustrate the correlations between intermolecular nonionic/zwitterionic associations and blood compatibility of PNIPAAm, PNIPAAm-b-PSBMA, and PSBMA suspension in human blood. Human fibrinogen adsorption onto the PNIPAAm-b-PSBMA copolymers from single-protein solutions was measured by DLS to determine the nonfouling stability of copolymer suspension. The new nonfouling nature of PNIPAAm-b-PSBMA copolymers was demonstrated to show extremely high anticoagulant activity and antihemolytic activity in human blood over a wide range of explored temperatures from 4 to 40 °C. The temperature-independent blood compatibility of nonionic/zwitterionic block copolymer along with their schizophrenic phase behavior in aqueous solution suggests their potential in blood-contacting applications.


Assuntos
Acrilamidas/química , Acrilamidas/síntese química , Materiais Biocompatíveis/síntese química , Eritrócitos/efeitos dos fármacos , Metacrilatos/síntese química , Polímeros/química , Acrilamidas/farmacologia , Resinas Acrílicas , Adsorção , Materiais Biocompatíveis/farmacologia , Eritrócitos/citologia , Fibrinogênio/química , Hemólise/efeitos dos fármacos , Humanos , Luz , Espectroscopia de Ressonância Magnética , Metacrilatos/farmacologia , Micelas , Peso Molecular , Nefelometria e Turbidimetria , Polimerização , Espalhamento a Baixo Ângulo , Soluções , Temperatura Ambiente , Água
3.
Langmuir ; 28(9): 4309-17, 2012 Mar 06.
Artigo em Inglês | MEDLINE | ID: mdl-22268580

RESUMO

In this work, bioadhesive behavior of plasma proteins and blood cells from umbilical cord blood (UCB) onto zwitterionic poly(sulfobetaine methacrylate) (polySBMA) polymer brushes was studied. The surface coverage of polySBMA brushes on a hydrophobic polystyrene (PS) well plate with surface grafting weights ranging from 0.02 mg/cm(2) to 0.69 mg/cm(2) can be effectively controlled using the ozone pretreatment and thermal-induced radical graft-polymerization. The chemical composition, grafting structure, surface hydrophilicity, and hydration capability of prepared polySBMA brushes were determined to illustrate the correlations between grafting properties and blood compatibility of zwitterionic-grafted surfaces in contact with human UCB. The protein adsorption of fibrinogen in single-protein solutions and at complex medium of 100% UCB plasma onto different polySBMA brushes with different grafting coverage was measured by enzyme-linked immunosorbent assay (ELISA) with monoclonal antibodies. The grafting density of the zwitterionic brushes greatly affects the PS surface, thus controlling the adsorption of fibrinogen, the adhesion of platelets, and the preservation of hematopoietic stem and progenitor cells (HSPCs) in UCB. The results showed that PS surfaces grafted with polySBMA brushes possess controllable hydration properties through the binding of water molecules, regulating the bioadhesive and bioinert characteristics of plasma proteins and blood platelets in UCB. Interestingly, it was found that the polySBMA brushes with an optimized grafting weight of approximately 0.1 mg/cm(2) at physiologic temperatures show significant hydrated chain flexibility and balanced hydrophilicity to provide the best preservation capacity for HSPCs stored in 100% UCB solution for 2 weeks. This work suggests that, through controlling grafting structures, the hemocompatible nature of grafted zwitterionic polymer brushes makes them well suited to the molecular design of regulated bioadhesive interfaces for use in the preservation of HSPCs from human UCB.


Assuntos
Células Sanguíneas/citologia , Proteínas Sanguíneas/química , Sangue Fetal/citologia , Polímeros/química , Adesividade , Materiais Biocompatíveis/química , Células Sanguíneas/metabolismo , Ensaio de Imunoadsorção Enzimática , Humanos , Metacrilatos/química , Propriedades de Superfície
4.
Langmuir ; 27(9): 5445-55, 2011 May 03.
Artigo em Inglês | MEDLINE | ID: mdl-21449586

RESUMO

In this work, the hemocompatibility of PEGylated poly(vinylidene fluoride) (PVDF) microporous membranes with varying grafting coverage and structures via plasma-induced surface PEGylation was studied. Network-like and brush-like PEGylated layers on PVDF membrane surfaces were achieved by low-pressure and atmospheric plasma treatment. The chemical composition, physical morphology, grafting structure, surface hydrophilicity, and hydration capability of prepared membranes were determined to illustrate the correlations between grafting qualities and hemocompatibility of PEGylated PVDF membranes in contact with human blood. Plasma protein adsorption onto different PEGylated PVDF membranes from single-protein solutions and the complex medium of 100% human plasma were measured by enzyme-linked immunosorbent assay (ELISA) with monoclonal antibodies. Hemocompatibility of the PEGylated membranes was evaluated by the antifouling property of platelet adhesion observed by scanning electron microscopy (SEM) and the anticoagulant activity of the blood coagulant determined by testing plasma-clotting time. The control of grafting structures of PEGylated layers highly regulates the PVDF membrane to resist the adsorption of plasma proteins, the adhesion of platelets, and the coagulation of human plasma. It was found that PVDF membranes grafted with brush-like PEGylated layers presented higher hydration capability with binding water molecules than with network-like PEGylated layers to improve the hemocompatible character of plasma protein and blood platelet resistance in human blood. This work suggests that the hemocompatible nature of grafted PEGylated polymers by controlling grafting structures gives them great potential in the molecular design of antithrombogenic membranes for use in human blood.


Assuntos
Materiais Biocompatíveis/química , Incrustação Biológica/prevenção & controle , Membranas Artificiais , Plasma/metabolismo , Polivinil/química , Atmosfera , Humanos , Propriedades de Superfície
5.
ACS Appl Mater Interfaces ; 3(4): 1228-37, 2011 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-21388227

RESUMO

Development of nonfouling membranes to prevent nonspecific protein adsorption and platelet adhesion is critical for many biomedical applications. It is always a challenge to control the surface graft copolymerization of a highly polar monomer from the highly hydrophobic surface of a fluoropolymer membrane. In this work, the blood compatibility of poly(vinylidene fluoride) (PVDF) membranes with surface-grafted electrically neutral zwitterionic poly(sulfobetaine methacrylate) (PSBMA), from atmospheric plasma-induced surface copolymerization, was studied. The effect of surface composition and graft morphology, electrical neutrality, hydrophilicity and hydration capability on blood compatibility of the membranes were determined. Blood compatibility of the zwitterionic PVDF membranes was systematically evaluated by plasma protein adsorption, platelet adhesion, plasma-clotting time, and blood cell hemolysis. It was found that the nonfouling nature and hydration capability of grafted PSBMA polymers can be effectively controlled by regulating the grafting coverage and charge balance of the PSBMA layer on the PVDF membrane surface. Even a slight charge bias in the grafted zwitterionic PSBMA layer can induce electrostatic interactions between proteins and the membrane surfaces, leading to surface protein adsorption, platelet activation, plasma clotting and blood cell hemolysis. Thus, the optimized PSBMA surface graft layer in overall charge neutrality has a high hydration capability and the best antifouling, anticoagulant, and antihemolytic activities when comes into contact with human blood.


Assuntos
Betaína/análogos & derivados , Sangue , Materiais Revestidos Biocompatíveis/química , Membranas/química , Polivinil/química , Betaína/química , Humanos , Teste de Materiais
6.
ACS Appl Mater Interfaces ; 2(12): 3642-7, 2010 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-21090586

RESUMO

Multiwalled carbon nanotubes functionalized with poly(sulfone) (PSF) and poly(sulfobetaine methacrylate) (PSBMA) (MWNT-PSF/PSBMA) have been prepared through sequential atom transfer radical polymerization. The structure of MWNT-PSF/PSBMA hybrid has been characterized with FTIR, Raman spectroscopy, and high-resolution transmission electron microscopy. Incorporation of PSBMA chains to MWNTs introduces amphiphilic and protein-resistant properties to MWNT-PSF/PSBMA. Addition of 1 wt % MWNT-PSF/PSBMA to PSF films significantly improves their protein-resistant characteristic, as the composite films show a 4.4% of protein adsorption compared to poly(styrene) Petri dishes. The PSF/MWNT-PSF/PSBMA composite has been applied to prepare antifouling ultrafiltration membranes for protein separation. This work demonstrates an effective and convenient approach to prepare low-protein-adsorption surfaces and antifouling membranes.


Assuntos
Membranas Artificiais , Metacrilatos/química , Nanotubos de Carbono/química , Nanotubos de Carbono/ultraestrutura , Polímeros/química , Proteínas/química , Sulfonas/química , Adsorção , Sítios de Ligação , Cristalização/métodos , Interações Hidrofóbicas e Hidrofílicas , Teste de Materiais , Membranas , Nanotecnologia/métodos , Tamanho da Partícula , Ligação Proteica
7.
Langmuir ; 26(22): 17286-94, 2010 Nov 16.
Artigo em Inglês | MEDLINE | ID: mdl-20882958

RESUMO

This work describes a tunable blood compatibility of zwitterionic poly(sulfobetaine methacrylate) (polySBMA) polymers at a wide range of high molecular weights from 50 kDa to 300 kDa controlled with a similar polydispersity via homogeneous free-radical polymerization. The control of molecular weights of polySBMA highly regulates the zwitterionic nonfouling nature to resist the adsorption of plasma proteins, the coagulant of human plasma, and the hemolysis of red blood cells. In this study, the upper critical solution temperatures (UCSTs) and hydrodynamic size of prepared polymers are determined to illustrate the correlations between intermolecular zwitterionic associations and blood compatibility of polySBMA suspension in human blood. The polySBMA exhibited clear shifts of UCSTs in the stimuli-responsive control of solution pH and ionic strength, which were strongly associated with the molecular weights of the prepared polymers. Plasma-protein adsorption onto the polySBMA polymers from single-protein solutions and the complex medium of 100% human plasma were measured by dynamic light scattering to determine the nonfouling stability of polySBMA suspension. It was found that the nonfouling nature as well as hydration capability of polySBMA can be effectively controlled via regulated molecular weights of zwitterionic polymers. This work shows that the polySBMA polymer with an optimized molecular weight of about 135 kDa at physiologic temperature is presented high hydration capability to function the best nonfouling character of anticoagulant activity and antihemolytic activity in human blood. The excellent blood compatibility of zwitterionic polySBMA along with their stimuli-responsive phase behavior in aqueous solution suggests their potential for use in blood-contacting targeted delivery and diagnostic applications.


Assuntos
Incrustação Biológica/prevenção & controle , Sangue/efeitos dos fármacos , Teste de Materiais/métodos , Metacrilatos/química , Metacrilatos/farmacologia , Água/química , Coagulação Sanguínea/efeitos dos fármacos , Proteínas Sanguíneas/química , Proteínas Sanguíneas/metabolismo , Humanos , Concentração de Íons de Hidrogênio , Metacrilatos/metabolismo , Peso Molecular , Concentração Osmolar , Contagem de Plaquetas , Soluções , Temperatura Ambiente
8.
Biomacromolecules ; 11(4): 1101-10, 2010 Apr 12.
Artigo em Inglês | MEDLINE | ID: mdl-20201492

RESUMO

This work describes a novel tunable bioadhesive hydrogel of thermoresponsive N-isopropylacrylamide (NIPAAm) containing zwitterionic sulfobetaine methacrylate (SBMA). This novel hydrogel highly regulates general bioadhesive foulants through the adsorption of plasma proteins, the adhesion of human platelets and cells, and the attachment of bacteria. In this investigation, nonionic hydrogels of polyNIPAAm, zwitterionic hydrogels of polySBMA, and three copolymeric hydrogels of NIPAAm and SBMA (poly(NIPAAm-co-SBMA)) were prepared. The copolymeric hydrogels exhibited controllable temperature-dependent swelling behaviors and showed stimuli-responsive phase characteristics in the presence of salts. The interactions of these hydrogels with biomolecules and microorganisms were demonstrated by protein adsorption, cell adhesion, and bacterial attachment, which allowed us to evaluate their bioadhesive properties. An enzyme-linked immunosorbent assay (ELISA) with monoclonal antibodies was used to measure different plasma protein adsorptions on the prepared hydrogel surfaces. At a physiological temperature, the high content of the nonionic polyNIPAAm in poly(NIPAAm-co-SBMA) hydrogel exhibits a high protein adsorption due to the interfacial exposure of polyNIPAAm-rich hydrophobic domains. A relatively high content of polySBMA in poly(NIPAAm-co-SBMA) hydrogel exhibits reduced amounts of protein adsorption due to the interfacial hydration of polySBMA-rich hydrophilic segments. The attachment of platelets and the spreading of cells were only observed on polyNIPAAm-rich hydrogel surfaces. Interestingly, the incorporation of zwitterionic SBMA units into the polyNIPAAm gels was found to accelerate the hydration of the cell-cultured surfaces and resulted in more rapid cell detachment. Such copolymer gel surface was shown to be potentially useful for triggered cell detachment. In addition, the interactions of hydrogels with bacteria were also evaluated. The polySBMA-rich hydrogels exhibited evident antimicrobial properties when they were incubated with Gram-positive bacteria ( S. epidermidis ) and Gram-negative bacteria ( E. coli ). This work shows that the bioadhesive properties of poly(NIPAAm-co-SBMA) hydrogels can be effectively controlled via regulated nonionic and zwitterionic molar mass ratios. The tunable-bioadhesive behavior of temperature-sensitive poly(NIPAAm-co-SBMA) makes this biocompatible hydrogel appropriate for biomedical applications.


Assuntos
Acrilamidas/química , Betaína/análogos & derivados , Materiais Biocompatíveis/química , Adesão Celular , Hidrogéis/química , Polímeros/química , Betaína/química , Materiais Biocompatíveis/síntese química , Materiais Biocompatíveis/metabolismo , Plaquetas/metabolismo , Proteínas Sanguíneas/metabolismo , Células Cultivadas , Escherichia coli/metabolismo , Fibroblastos/metabolismo , Humanos , Polímeros/síntese química , Polímeros/metabolismo , Staphylococcus epidermidis/metabolismo , Propriedades de Superfície , Temperatura Ambiente
9.
Langmuir ; 26(5): 3522-30, 2010 Mar 02.
Artigo em Inglês | MEDLINE | ID: mdl-19947616

RESUMO

In this work, the hemocompatibility of a sulfobetaine-like copolymer brush resulting from a mixed-charge copolymerization of the positively charged 11-mercapto-N,N,N-trimethylammonium chloride (TMA) and negatively charged 11-mercaptoundecylsulfonic acid (SA) was studied. Mixed charge distribution in the prepared poly(TMA-co-SA) copolymer brushes was controlled by the regulation of the reaction rate of the surface-initiated atom transfer radical polymerization (ATRP). The adsorption behavior of plasma proteins on a surface grafted with poly(TMA-co-SA) was measured by a surface plasmon resonance (SPR) sensor. The effects of varying temperature, solution pH, and ionic strength on the antifouling characteristics of the mixed-charge copolymer brushes were systematically evaluated, and the protein-fouling resistance was discussed in detail, especially with respect to the effect of ionic strength on the intra- and intermolecular interactions of the poly(TMA-co-SA) with proteins. The adhesion and activation of blood cells on the poly(TMA-co-SA)-grafted surface in contact with human whole blood was also demonstrated. The results suggest that mixed-charge copolymer brushes of poly(TMA-co-SA), which, like zwitterionic homopolymer brushes, have overall charge neutrality, can be used in similar applications for protein-fouling resistance and have excellent hemocompatibility with human whole blood at physiologic temperatures.


Assuntos
Materiais Biocompatíveis/química , Incrustação Biológica , Proteínas Sanguíneas/química , Polímeros/química , Compostos de Amônio Quaternário/química , Compostos de Sulfidrila/química , Adsorção , Materiais Biocompatíveis/síntese química , Células Sanguíneas/citologia , Adesão Celular , Humanos , Concentração de Íons de Hidrogênio , Concentração Osmolar , Polímeros/síntese química , Temperatura Ambiente
10.
Biomacromolecules ; 10(8): 2092-100, 2009 Aug 10.
Artigo em Inglês | MEDLINE | ID: mdl-19572632

RESUMO

Thermoresponsive statistical copolymers of zwitterionic sulfobetaine methacrylate (SBMA) and nonionic N-isopropylacrylamide (NIPAAm) were prepared with an average molecular weight of about 6.0 kDa via homogeneous free radical copolymerization. The aqueous solution properties of poly(SBMA-co-NIPAAm) were measured using a UV--visible spectrophotometer. The copolymers exhibited controllable lower and upper critical solution temperatures in aqueous solution and showed stimuli-responsive phase transition in the presence of salts. Regulated zwitterionic and nonionic molar mass ratios led to poly(SBMA-co-NIPAAm) copolymers having double-critical solution temperatures, where the water-insoluble polymer microdomains are generated by the zwitterionic copolymer region of polySBMA or nonionic copolymer region of polyNIPAAm depending on temperature. A high content of the nonionic polyNIPAAm in poly(SBMA-co-NIPAAm) exhibits nonionic aggregation at high temperatures due to the desolvation of polyNIPAAm, whereas relatively low content of polyNIPAAm in poly(SBMA-co-NIPAAm) exhibits zwitterionic aggregation at low temperatures due to the desolvation of polySBMA. Plasma protein adsorption on the surface coated with poly(SBMA-co-NIPAAm) was measured with a surface plasmon resonance (SPR) sensor. The copolymers containing polySBMA above 29 mol % showed extremely low protein adsorption and high anticoagulant activity in human blood plasma. The tunable and switchable thermoresponsive phase behavior of poly(SBMA-co-NIPAAm), as well as its high plasma protein adsorption resistance and anticoagulant activity, suggests a potential for blood-contacting applications.


Assuntos
Acrilamidas/química , Anticoagulantes/química , Materiais Biocompatíveis/química , Proteínas Sanguíneas/química , Polímeros/química , Ouro/química , Humanos , Transição de Fase , Ressonância de Plasmônio de Superfície , Propriedades de Superfície , Temperatura Ambiente
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