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At least 523 records · Page 29Linked to original sources
PubMed1998

Identification of a blue photoluminescent composite material from a combinatorial library

A quaternary combinatorial masking strategy was used in conjunction with photolithography to generate compositionally diverse thin-film phosphor libraries containing 1024 different compositions on substrates 2.5 centimeters square. A parallel imaging system and scanning spectrophotometer were used to identify and characterize compositions in the library with interesting luminescent behavior. Optimal compositions were identified with the use of gradient libraries, in which the stoichiometry of a material was varied continuously. This process led to the identification of an efficient blue photoluminescent composite material, Gd3Ga5O12/SiO2. Experimental evidence suggests that luminescence in this material may arise from interfacial effects between SiO2 and Gd3Ga5O12.

Journal Article↗
PubMed1991

SEM and energy dispersive X-ray surface analysis of the interfacial region of selected porcelain-metal systems.

Comparative bond strength data of Ceramco and Vita opaque and body porcelains when fired to high noble, medium noble, and base metal porcelain-fused-to-metal alloys were recently published. In the present study SEM and energy dispersive X-ray (EDX) microanalyses were undertaken--using the same specimens after debonding--to relate the bond strengths reported for 12 different porcelain-metal composites to morphology and chemistry at fracture sites. SEM examination revealed intimate contact between the different porcelains and the metal oxide substrates. On Olympia, a medium noble alloy, bubbles trapped in porcelain at or near fracture sites appeared to decrease the potential interaction. Area scan semiquantitative EDX analysis of the interfacial fracture sites detected high concentrations of metal oxides thought to be essential for a successful chemical bond. Multi-spot surface spectroscopy on similar traces of porcelain residuals revealed significant differences in the amount of particular back scattering activity. Further examination with cross sectional quantitative EDX analysis is suggested for a more precise characterization of element concentration within all components of the porcelain-metal interface.

Dental Alloys↗
PubMed1984

Molecular mechanisms of gossypol action on lipid membranes.

Gossypol, an aldehyde extracted from cotton plants, produces both general toxic and antifertility effects in mammals. The cellular mechanisms by which gossypol exerts these effects are not understood. In this study, we have characterized the interactions of gossypol with lipid monolayer and bilayer membranes in order to assess if the drug acts by modifying the electrochemical properties of membranes. The charged form of gossypol binds to monolayers of different lipid compositions with apparent dissociation constants ranging from 0.7 to 2 microM. Binding of charged gossypol decreases the interfacial potential by 80-235 mV, the magnitude of this decrease being dependent upon the lipid composition. Gossypol also induces a conductance in phospholipid bilayer membranes. The relation between steady-state bilayer conductance versus gossypol concentration indicates that the current-carrying species is a single molecule of gossypol. The increase in bilayer conductance is accompanied by an increase in proton permeability. These changes induced by gossypol in model membranes can account for the mitochondrial uncoupling effects of this molecule and may be responsible for the inhibitory effects of gossypol on several membrane transport systems.

Animals↗
PubMed2005

Structure, function and interfacial allosterism in phospholipase A2: insight from the anion-assisted dimer.

Enzymes that function on membrane surfaces offer many challenges to understanding structural and functional details due to the difficulties of obtaining relevant information of the protein in a physiological environment. Focusing on this aspect of structural biology, it is important to develop conditions that mimic the interaction of membrane proteins with their binding surface and ultimately the mechanisms of action. This approach has been used to characterize the allosteric nature of secreted phospholipase A2 (PLA2) to its substrate interface. The breakthrough here was to crystallize the pancreatic group-IB PLA2 in an anion-assisted dimer with five coplanar phosphate anions bound. In the anion-assisted dimer structure one molecule of a tetrahedral mimic inhibitor and five anions are shared between the two subunits of the dimer. The sn-2-phosphate of the inhibitor, which mimics the tetrahedral intermediate of the esterolysis reaction, is bound in the active site of one subunit, and the alkyl chain extends into the active site slot of the second subunit across the subunit-subunit interface. This interface-bound structural mimic provided insight into the active site environment and specific anionic interactions to the i-face of the protein. The presence or absence of a single critical active site water, corresponds to the difference between the activated or inactivated form of the enzyme. The anion-assisted dimer structure supports a calcium coordinated nucleophilic water mechanism, with its pK(a) modulated by this assisting water. This working model has been further strengthened with an enzyme-product complex structure solved with the hydrolysis products of the substrate PAF also bound to the anion-assisted dimer form of PLA2. Additional confirmation of the assisting-water mechanism comes from a structure of the inactive zymogen proPLA2 also crystallized in an anion-assisted dimer. Remarkably, the assisting water present in the activated complex is absent in this proPLA2 structure.

Allosteric Site↗
PubMed2005

Characterization and histochemical localization of nonspecific esterase from ascocarps of desert truffle (Terfezia claveryi Chatin).

An esterase activity from Terfezia claveryi Chatin ascocarps, a mycorrhizal hypogeous fungus, is described for the first time. The enzyme was partially purified using phase partitioning in Triton X-114 (TX-114), achieving a reduction of 87% in the triglyceride content and the removal of 63% of phenols. The enzyme showed maximum activity toward short-chain p-nitrophenyl esters, and no interfacial activation was observed, indicating that the enzyme responsible for this activity is an esterase and not a lipase. This esterase presented its maximum activity at pH 7.4 and 60 degrees C. The values obtained for Km at pH 7.4 were 0.3 mM for p-nitrophenyl butyrate and 0.6 mM for p-nitrophenyl acetate with catalytic efficiencies (Vmax/Km) of 0.23 and 0.32, respectively. T. claveryi esterase was inhibited by phenylboric acid, indicating that serine residues were involved in the enzyme activity. This activity was localized only in the hypothecium and was absent from the peridium and gleba.

Ascomycota↗
PubMed2005

Investigation of the core-shell interface in gold@silica nanoparticles: a silica imprinting approach.

The nature of the self-assembled core-shell interface in gold@silica nanoparticles synthesized via a 3-aminopropyltrimethoxysilane (APTMS) route is investigated using materials synthesis as a sensitive tool for elucidating interfacial composition and organization. Our approach involves condensation of the gold@silica nanoparticles within a silica framework for synthesis of a composite gold-silica material containing approximately 30 wt % gold. This material contains one of the highest gold loadings reported, but maintains gold core isolation as ascertained via a single surface plasmon resonance absorption band frequency corresponding to that of gold nanoparticles in dilute aqueous solution. The immobilized gold cores are subsequently etched using cyanide anion for the synthesis of templated porosity, which corresponds to the space that was occupied by the gold. Characterization of immobilized amines is performed using probe molecule binding experiments, which demonstrate a lack of accessible amines after gold removal. Solid-state 13C CPMAS NMR spectroscopy on these materials demonstrates that the amount of amine immobilization must be less than 10% of the expected yield, assuming that all of the APTMS becomes bound to the gold nanoparticle template. These results require a core-shell interface in the gold@silica nanoparticles that is predominantly occupied by inorganic silicate species, such as Si-O-Si and Si-OH, rather than primary amines. Such a result is likely a consequence of the weak interaction between primary amines and gold in aqueous solution. Our method for investigating the core-shell interface of gold@silica nanoparticles is generalizable for other interfacial structures and enables the synthesis of bulk imprinted silica using colloidal templates.

Journal Article↗
PubMed2005

Voltammetric investigation of cytochrome c on gold coated with a self-assembled glutathione monolayer.

The direct, reversible electrochemistry of horse-heart cytochrome c (cyt. c) was realized on a self-assembled glutathione (GSH) monolayer modified Au electrode. The voltammetric responses of cyt. c on GSH/Au electrode were found to be affected by pH during the electrode modification, metal ions and surfactants. Using potassium ferricyanide [K4Fe(CN)6] as a probe, these effects on the voltammetric responses of cyt. c were characterized by electrochemical methods. It was found that the pH during the electrode modification, metallic ions and surfactants changed GSH monolayer's charge state and the conformation on the electrode surface, and resulted in the influence on the voltammetric responses of cyt. c. The experimental results provided us information to understand the mechanism of the interfacial electron transfer of electrode-protein, as well as the electron transfer of cyt. c in life system.

Animals↗
PubMed2006

Surface interactions of s-triazine-type pesticides. An electrochemical impedance study.

Two pesticides, atrazine and terbutylazine, have very similar chemical structures differing only by iso-propyl and tert-butyl substituents on their 6 amino groups. This minor structural difference causes profound effects in decomposition rates in the environment, leading to a ban of atrazine in the European Union. Here we present a study of adsorption at ideally polarized electrochemical interface in the absence of specifically adsorbed halides. The interfacial charge and the temperature determine which type of an adsorbed film is formed. The double layer capacitance measurements yield the critical temperature of the surface film transition, which is markedly different for the two pesticides. The time-resolved impedance spectroscopy indicates slow changes within the film structure that becomes disordered and can be characterized in terms of the fractal geometry.

Journal Article↗
PubMed1979

Glycerolipid and Fatty Acid Changes in Eastern White Pine Chloroplast Lamellae during the Onset of Winter.

Chloroplast lamellae of eastern white pine (Pinus strobus L.) were analyzed to determine changes in total glycerolipids, component glycerolipids, and glycerolipid fatty acids during the onset of winter hardiness. Samples were collected in September, November, and December when the average daily temperature varied between 23 and -10 C. Before November 2, phospholipids decreased 40 to 85%, glycolipids only 30%. Analysis of individual glycerolipids showed that glycerolipids containing 18:3 fatty acid were retained at the expense of glycerolipids esterified with saturated (16:0 and 18:0) and monounsaturated (18:1) fatty acids.Between mid-November and December, the total quantity of lamellar glycerolipids recovered to the September level. Increases in digalactosyl diglyceride and in 18:3 characterized the recovery period. High lamellar unsaturation achieved by mid-November appeared to be maintained during recovery through preferential incorporation of glycerolipids containing 18:3 (monogalactosyl diglyceride, digalactosyl diglyceride, phosphatidylglycerol, and phosphatidylcholine).These results suggest that eastern white pine chloroplasts maintain lamellar viscosity by increasing lamellar unsaturation and tolerate freeze desiccation by increasing the interfacial water-binding capacity of the lamellae.

Journal Article↗
PubMed2001

Enzyme-modulated cleavage of dsDNA for studying interfacial biomolecular interactions.

This work describes the chemistry and methodology for constructing multilayers of bis-biotinylated dsDNA on metal substrates after enzyme cleavage and demonstrates its use for amplified microgravimetric and impedimetric analyses of anticancer drug, cisplatin. Specific chemical modification of dsDNA prior to immobilization was achieved via a bisulfite-catalyzed transamination of cytosine after endonuclease cleavage of plasmid DNA. The specificity of the reaction of cytosine residues at ss- versus dsDNA loci after endonuclease cleavage was characterized using circular dichroism, mass spectrometry, and absorption spectrophotometry. The biotinylated dsDNA consisting of 2961 base pairs was then used as a ligand at avidin-modified gold electrodes. Ac impedance spectroscopy and quartz crystal microbalance measurements clearly showed that the response to cisplatin increased linearly with target concentrations. The impedance spectroscopy resulted in a detection limit of 1 nM and a surface density of 4.8 x 10(13) molecules/0.1 cm(2). The immobilization of dsDNA on surfaces is a significant improvement over existing approaches in that it enables the attachment of long pieces of unmodified double-stranded DNA via a simple biotinylation step. The immobilization technique provides a generic approach for dsDNA-based sensor development and for monitoring DNA-analyte interactions.

Biotin↗
PubMed2005

Cross linking and rheological characterization of adsorbed protein layers at the oil-water interface.

The dilatational rheological properties of cross-linked protein layers adsorbed at the oil-water interface were investigated with help of a modified drop tensiometer allowing successive replacements of the external phase. This setup enables one to perform cross-linking reactions at the interface only, that is, without any contact between the cross-linking agent and protein molecules in solution, under continuous monitoring of the interfacial tension. The mechanical properties of the resulting interface were investigated with dilatational large strain experiments. Measured rheological properties were related to the expected stability of an emulsion against disproportionation by considering the ratio of the interfacial elasticity to the interfacial tension. In an attempt to increase this ratio to improve the resistance against disproportionation, experiments were performed with densified protein layers obtained via reduction of the droplet area prior to cross linking. To highlight the influence of the protein morphology on the dilatational rheological properties of the cross-linked adsorbed layers, experiments were performed with random coil (beta-casein) as well as globular (beta-lactoglobulin) proteins. Glutaraldehyde was used as a cross-linking agent. Experiments were performed at 55 degrees C and pH 7.0 in 20 mM imidazole buffer for later comparison with enzymatically cross-linked adsorbed protein layers. The present work demonstrated substantial qualitative and quantitative differences in the interfacial rheological properties of cross-linked random coil and globular proteins.

Adsorption↗
PubMedDate not supplied

Production of starch foams by twin-screw extrusion: effect of maleated poly(butylene adipate-co-terephthalate) as a compatibilizer.

Free-radical-initiated grafting of maleic anhydride (MA) onto poly(butylene adipate-co-terephthalate) (PBAT), a biodegradable aliphatic-aromatic copolyester, was performed by reactive extrusion. 2,5-Dimethyl-2,5-di(tert-butylperoxy)hexane was used as the free-radical initiator. The peroxide concentration was varied between 0.0 and 0.5 wt % at 3.0 wt % MA concentration; the MA concentration was varied between 1.0 and 5.0 wt % at 0.5 wt % peroxide concentration. The reaction temperature was maintained at 185 degrees C for all experiments. Under these conditions, between 0.194% and 0.691% MA was grafted onto the polyester backbone. Size-exclusion chromatography, melt flow index, intrinsic viscosity measurements, thermal gravimetric analysis, and differential scanning calorimetry were used to characterize the maleated copolyester. Increasing the initiator concentration at a constant MA concentration of 3% resulted in an increase in the grafting of MA while decreasing the molecular weight of the resulting polymer. Increasing the feed MA concentration also increased the grafting percentage. The maleation of the polyester proved to be very efficient in promoting strong interfacial adhesion with high amylose cornstarch in starch foams as prepared by melt blending. Thus, the use of maleated copolyester as a compatibilizer between starch and PBAT allowed the reduction of the density of resulting starch foams to approximately 21 kg/m3 and improved the resilience from 84% to as high as 95%. Also, the resulting starch foams exhibited improved hydrophobic properties in terms of lower weight gain and higher dimensional stability on moisture sorption.

Biodegradation, Environmental↗
PubMed2006

Gradual change or phase transition: characterizing fluid lipid-cholesterol membranes on the basis of thermal volume changes.

Cholesterol has been reported to govern biomembrane permeability, elasticity, and the formation of lipid rafts. There has been a controversy whether binary lipid-cholesterol membranes should better be described in terms of a phase separation (liquid-ordered and liquid-disordered phases) or of gradual changes in largely homogeneous membranes. We present a new approach for detecting and characterizing phase equilibria in colloidal dispersions using pressure perturbation calorimetry (PPC). We apply this to the study of the thermal expansivity of mixtures of 1-palmitoyl-2-oleoyl sn-glycero-3-phosphatidylcholine (POPC) and cholesterol as a function of composition and temperature. We show that cholesterol can condense lipids not only laterally (with respect to interfacial area) but also in volume. A quantitative comparison with expansivity curves simulated assuming either phase separation or random mixing within one phase reveals that the real system shows an intermediate behavior due to submicroscopic demixing effects. However, both models yield consistent system parameters and are thus found to be useful for describing the systems to a similar approximation. Accordingly, one cholesterol may condense 3 +/- 1 1-palmitoyl-2-oleoyl-sn-glycero-3-phosphatidylcholine molecules by approximately -(1.4 +/- 0.5) vol % at 2 degrees C; both absolute values decrease with increasing temperature.

Calorimetry↗
PubMed2006

Laser ultrasonic characterization of adhesive bonds between epoxy coating and aluminum substrate.

Nanosecond pulsed laser irradiation through transparent epoxy bonded to aluminum substrate excites wide-band ultrasonic waves at the bonded interface. The normal displacements on the rear surface of aluminum produced by the direct and multi-reflected longitudinal waves in the coating layer are detected by a laser interferometer. The amplitude of the reflected signal depends on the properties of the coating/substrate interface, which is described by terms of the interfacial stiffness using a spring boundary model. The waveforms at the epicenter versus interfacial stiffness are simulated and found to be in good agreement with experimental results. The relation between the interfacial stiffness and the amplitude ratio of the reflected and direct waves is thus established. An image of amplitude ratio of a specimen (null 10 mm) is obtained from the epicenter waveforms recorded by a laser ultrasonic scanning system, which shows the distribution of bond quality on the bonding interface.

Journal Article↗
PubMed2000

Supported membranes on soft polymer cushions: fabrication, characterization and applications.

Soft biofunctional and biocompatible interfaces on solids designed by the deposition of ultrathin soft polymer films or supported membranes have numerous scientific and practical applications. These include the immobilization of glycolipids, membrane receptors and proteins to generate models of cell and tissue surfaces. Powerful surface-sensitive techniques can be applied to study protein-protein recognition processes at membranes and the control of cell adhesion by the interplay of specific 'lock-and-key' forces and universal interfacial forces. Potential practical applications include the design of smart biosensors based on electro-optical devices and the fabrication of biofunctional surfaces for the stimulation of cell proliferation and tissue growth, or for the suppression of apoptosis.

Biosensing Techniques↗
PubMed1999

A specific human lysophospholipase: cDNA cloning, tissue distribution and kinetic characterization.

Lysophospholipases are critical enzymes that act on biological membranes to regulate the multifunctional lysophospholipids; increased levels of lysophospholipids are associated with a host of diseases. Herein we report the cDNA cloning of a human brain 25 kDa lysophospholipid-specific lysophospholipase (hLysoPLA). The enzyme (at both mRNA and protein levels) is widely distributed in tissues, but with quite different abundances. The hLysoPLA hydrolyzes lysophosphatidylcholine in both monomeric and micellar forms, and exhibits apparent cooperativity and surface dilution kinetics, but not interfacial activation. Detailed kinetic analysis indicates that the hLysoPLA binds first to the micellar surface and then to the substrate presented on the surface. The kinetic parameters associated with this surface dilution kinetic model are reported, and it is concluded that hLysoPLA has a single substrate binding site and a surface recognition site. The apparent cooperativity observed is likely due to the change of substrate presentation. In contrast to many non-specific lipolytic enzymes that exhibit lysophospholipase activity, hLysoPLA hydrolyzes only lysophospholipids and has no other significant enzymatic activity. Of special interest, hLysoPLA does not act on plasmenylcholine. Of the several inhibitors tested, only methyl arachidonyl fluorophosphonate (MAFP) potently and irreversibly inhibits the enzymatic activity. The inhibition by MAFP is consistent with the catalytic mechanism proposed for the enzyme - a serine hydrolase with a catalytic triad composed of Ser-119, Asp-174 and His-208.

Amino Acid Sequence↗
PubMed2003

Synthesis and characterization of a novel polymer-ceramic system for biodegradable composite applications.

The objective of this study was to develop a biodegradable polymer resin that could be used for the fabrication of an interpenetrating phase composite (IPC) made of porous calcium polyphosphate (CPP) and an organic polymer resin. The resin was synthesized from a polycarbonate-based divinyl oligomer and monomers containing ionic groups. The physical and chemical properties of the polymer resin and polycarbonate-based divinyl oligomer were characterized by gel permeation chromatography, Fourier transform infrared spectroscopy, and swelling studies. The in vitro degradation of the polymer resins was assessed using cholesterol esterase in a buffer solution at 37 degrees C for 3 weeks. Scanning electron microscopy of the degraded samples indicated that the hydrolysis of the resin was catalyzed by the enzyme. The relative interfacial shear strength between the polymer resin and the CPP ceramic was studied using a microbond test. The addition of ionic groups into the polymer resin chains appeared to improve the chemical bonding between the polymer and the CPP. Preliminary mechanical properties of the IPC were investigated by determining bending strength using a three point bending test. The data showed a sevenfold increase in strength over that of the monolithic CPP, and the addition of more ionic groups into the resin led to a higher bending strength for the newly formed CPP/polycarbonate resin system. Sample cross sections of the IPC examined using scanning electron microscopy suggested that the resin had infiltrated almost all of the pores of the CPP. The results of this study indicate that the IPC could potentially be used for fabricating novel biodegradable load-bearing implants.

Biocompatible Materials↗
PubMed1992

Characterization of a bovine synovial fluid lubricating factor. I. Chemical, surface activity and lubricating properties.

A lubricating glycoprotein (PSLF) with an apparent molecular weight of 280 kDa was purified from bovine synovial fluid by anion exchange, molecular sieve chromatography, and density gradient centrifugation. Lubrication was measured under boundary conditions as lowering of the coefficient of friction (mu) between oscillating natural latex and polished glass. Lubricating ability was first observed at a concentration of 200 micrograms/ml and became maximal at 260 micrograms/ml. Hydrophobic interfacial tension measurements indicated that at the former concentration, monolayers of PSLF formed. Sugar digestions showed that lubricating ability depends upon the terminal galactose of the molecule. PSLF is similar if not identical to lubricin. It is proposed that a repulsive hydration force is the molecular mechanism for lubricating activity.

Amino Acids↗