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PubMed2001

Gas/solid partitioning of semivolatile organic compounds (SOCs) to air filters. 3. An analysis of gas adsorption artifacts in measurements of atmospheric SOCs and organic carbon (OC). WHen using teflon membrane filters and quartz fiber filters.

Adsorption of gaseous semivolatile organic compounds (SOCs) onto the filter(s) of a filter/sorbent sampler is a potential source of measurement error when determining specific SOCs as well as organic carbon (OC) levels in the atmosphere. This work examines partitioning to both Teflon membrane filters (TMFs) and quartz fiber filters (QFFs) for purposes of predicting the magnitude of the compound-dependent gas adsorption artifact as a function of various sampling parameters. The examination is based on values of Kp,face (m3 cm(-2)), the gas/filter partition coefficient expressed as [ng sorbed per cm2 of filter face]/[ng per m3 in the gas phase]. Values of Kp,face were calculated based on literature values of the gas/solid partition coefficient Kp,s [ng sorbed per m2 of filter]/[ng per m3 in gas phase] for the adsorption of various polycyclic aromatic hydrocarbons (PAHs), polychlorinated dibenzodioxins (PCDDs), and polychlorinated dibenzofurans (PCDFs) to TMFs, and for the adsorption of PAHs to QFFs. At relative humidity (RH) values below approximately 50%, the Kp,face values for PAHs are lower on TMFs than on ambient-backup QFFs. The gas adsorption artifact will therefore be lower for PAHs with TMFs than with QFFs under these conditions. In the past, corrections for the gas/filter adsorption artifact have been made by using a backup filter, and subtracting the mass amount of each compound found on the backup filter from the total (particle phase + sorbed on filter) amount found on the front filter. This procedure assumes that the ng cm(-2) amounts of each SOC sorbed on the front and backup filters are equal. That assumption will only be valid after both filters have reached equilibrium with each of the gaseous SOCs in the incoming sample air. The front filter will reach equilibrium first. The minimum air sample volume Vmin,f+b required to reach gas/filter sorption equilibrium with a pair of filters is 2Kp,face Afilter where Afilter (cm2) is the per-filter face area. Kp,face values, and therefore Vmin,f+b values, depend on the compound, relative humidity (RH), temperature, and filter type. Compound-dependent Vmin,f+b values are presented for PAHs and PCDD/Fs on both TMFs and QFFs. Compound-dependent equations which give the magnitude of the filter adsorption artifact are presented for a range of different sampling arrangements and circumstances. The equations are not intended for use in actually correcting field data because of uncertainties in actual field values of relevant parameters such as the compound-dependent Kp,face and gas/particle Kp values, and because of the fact that the equations assume ideal step-function chromatographic movement of gas-phase compounds through the adsorbing filter. Rather, the main utility of the equations is as guidance tools in designing field sampling efforts that utilize filter/sorbent samplers and in evaluating prior work. The results indicate that some backup-filter-based corrections described in the literature were carried out using sample volumes that were too small to allow proper correction for the gas adsorption artifactfor some specific SOCs of interest. Similar conclusions are reached regarding artifacts associated with the measurement of gaseous and particulate OC.

Adsorption↗
PubMed2001

Chlorothalonil and its 4-hydroxy derivative in simple quartz sand soils: a comparison of sorption processes.

Quartz sandy soils from Simcoe, Ontario, Canada and North Carolina had sorption properties for chlorothalonil that were nearly the same. For labile surface sorption kinetics, the Simcoe soil gave a pseudo first-order rate constant of kS1 = (7.4 +/- 0.7) x 10(-2) days-1. At equilibrium, the labile surface sorption capacity theta c of Simcoe soil for chlorothalonil was 23.8 x 10(-6) (mol/g). The sorption properties of the 4-hydroxy derivative of chlorothalonil were different in two important respects. They were larger by an order of magnitude, and they were substantially different for the two soils. Sorption by the Simcoe soil was too fast for kinetics measurements by the on-line HPLC micro extraction method, but for the North Carolina soil kS1 = (1.15 +/- 0.01) days-1 was recorded. For the Simcoe and North Carolina soils, respectively, theta c > 200 (mumol/g) and theta c approximately 113 (mumol/g). Two conclusions can be drawn. First, the replacement of the Cl by OH on the 4 position of chlorothalonil makes the sorption effects much greater. Second, the stronger interactions are associated with a greater sensitivity to small differences in the chemical compositions of the soils. Subtle soil properties causing significant effects might include small amounts and physical structures of organic matter and metal oxides. This implies that, for predictive computer models, mechanism parameters will have to be correlated in two dimensions: chemical structure, and the composition and amounts of chemical materials in soils.

Adsorption↗
PubMed2006

Monitoring and estimation of the kinetics parameters in the binding process of tannic acid to bovine serum albumin with electrochemical quartz crystal impedance system.

Combined measurements of piezoelectric quartz crystal impedance (PQCI) and electrochemical impedance (EI) were utilized in situ to monitor the adsorption of bovine serum albumin (BSA) onto the newly prepared Au colloid-modified electrode and study the binding process of tannic acid (TA) to BSA on the BSA-modified electrode surface. The time courses of the resonant frequency and the equivalent parameters of the sensor were simultaneously obtained during BSA adsorption and TA-BSA binding. Compared with the bare gold electrode, the Au colloid-modified gold electrode showed better biocompatibility, and the absorption capacity for BSA was increased by approximately 2.4 times. The observed frequency decrease was ascribed to the mass increase of the sensor surface resulting from the TA-BSA binding, which is believed to result mainly from the hydrogen bonding from FT-IR characterization. The maximal molar binding ratio of TA binding to immobilized BSA obtained from the frequency shift of the adsorbed BSA and TA was estimated to be 10.3:1. On the basis of the frequency decrease with time, the kinetics of the binding was quantitatively studied. By way of fitting the experimental data, the kinetics parameters, that is, binding and dissociation constant (k1, k(-1)), and the binding equilibrium constant (ka) were determined, giving values of 9.51 x 10(4) M(-1) s(-1), 3.15 s(-1), and 3.1 x 10(4) M(-1), respectively.

Electric Impedance↗
PubMed2006

Molecular modeling of interactions between L-lysine and functionalized quartz surfaces.

Molecular modeling techniques have been used to investigate the interaction of L-lysine in aqueous medium with silanol and methyl sites onto quartz substrates. The substrate effect has been studied for partially hydrophilic surfaces formed by silanol and methyl groups with a ratio of 1:5 and hydrophobic fully methylated surfaces. Molecular dynamics and static calculations indicate that L-lysine does not show any significant interaction with fully methylated surfaces, while its interaction with hydroxylated/methylated surfaces is dominated by electrostatic and H-bond terms. Accordingly, on fully methylated surfaces there is no preferential orientation of L-lysine with respect to the surface, while for hydroxylated/methylated surfaces the L-lysine-surface interaction mainly depends on the molecular orientation, with a preferred geometry involving the ammonium group pointing toward the silanol site. The structure of water shells around L-lysine molecules was shown to be strongly affected by the relative hydrophilic/hydrophobic character of the surfaces. In particular, the order is almost completely lost for partially hydrophilic surfaces, while well-defined hydration shells around L-lysine are obtained for hydrophobic surfaces.

Adsorption↗
PubMed2005

Dissipation-enhanced quartz crystal microbalance studies on the experimental parameters controlling the formation of supported lipid bilayers.

We report on the investigations of the transformation of spherically closed lipid bilayers to supported lipid bilayers in aqueous media in contact with SiO(2) surfaces. The adsorption kinetics of small unilamellar vesicles composed of dimyristoyl- (DMPC) and dipalmitoylphosphatidylcholine (DPPC) mixtures on SiO(2) surfaces were investigated using a dissipation-enhanced quartz crystal microbalance (QCM-D) as a function of buffer (composition and pH), lipid concentration (0.01-1.0 mg/mL), temperature (15-37 degrees C), and lipid composition (DMPC and DMPC/DPPC mixtures). The lipid mixtures used here possess a phase transition temperature (T(m)) of 24-33 degrees C, which is close to the ambient temperature or above and thus considerably higher than most other systems studied by QCM-D. With HEPES or Tris.HCl containing sodium chloride (150 mM) and/or calcium chloride (2 mM), intact vesicles adsorb on the surface until a critical density ((c)) is reached. At close vesicle contact the transformation from vesicles to supported phospholipid bilayers (SPBs) occurs. In absence of CaCl(2), the kinetics of the SPB formation process are slowed, but the passage through (c) is still observed. The latter disappears when buffers with low ionic strength were used. SPB formation was studied in a pH range of 3-10, yet the passage through (c) is obtained only for pH values above to the physiological pH (7.4-10). With an increasing vesicle concentration, (c) is reached after shorter exposure times. At a vesicle concentration of 0.01-1 mg/mL, vesicle fusion on SiO(2) proceeds with the same pathway and accelerates roughly proportionally. In contrast, the pathway of vesicle fusion is strongly influenced by the temperature in the vicinity of T(m). Above and around the T(m), transformation of vesicles to SPB proceeds smoothly, while below, a large number of nonruptured vesicles coexist with SPB. As expected, the physical state of the membrane controls the interaction with both surface and neighboring vesicles.

1,2-Dipalmitoylphosphatidylcholine↗
PubMed2006

Interaction between myoglobin and hyaluronic acid in their layer-by-layer assembly: quartz crystal microbalance and cyclic voltammetry studies.

Myoglobin (Mb), with different net surface charges at different pH in buffers and negatively charged hyaluronic acid (HA) at pH 5.0 in solutions were alternately adsorbed onto various solid surfaces and successfully assembled into {Mb/HA}(n) layer-by-layer films. The Mb in {Mb/HA}(n) films showed a quasi-reversible cyclic voltammetry (CV) response for its heme Fe(III)/Fe(II) redox couple. Quartz crystal microbalance (QCM) and CV were used to confirm the film growth and characterize the films. The interaction between Mb and HA and the influencing factors for Mb adsorption on HA surface, such as pH, Mb concentration, and ionic strength, were investigated in detail. The assembly driving force for {Mb/HA}(n) films, especially for the films assembled with like-charged Mb and HA, was found to be of electrostatic origin, while the secondary interaction such as hydrophobic interaction also plays an important role in some circumstances. Although the growth of {Mb(pH 7.0)/HA}(n) and {Mb(pH 9.0)/HA}(n) films was linear with the adsorption step, the exponential growth of {Mb(pH 5.0)/HA}(n) films was observed, especially when the films became thick. This exponential increase of mass and thickness with deposition step for {Mb(pH 5.0)/HA}(n) films was most probably attributed to the diffusion mechanism in which some HA molecules could diffuse in to and out of the whole films during the film assembly. Atomic force microscopy (AFM) results supported this speculation. UV-vis and IR spectroscopies of {Mb/HA}(n) films, combined with the comparative CV experiments of {Mb/HA}(n) and {catalase/HA}(n) films, suggest that Mb in the {Mb/HA}(n) multilayer films retains its near-native structure.

Adsorption↗
PubMed2006

Quantification of surface-bound proteins by fluorometric assay: Comparison with quartz crystal microbalance and amido black assay.

Protein adsorption is of major and widespread interest, being useful in the fundamental understanding of biological processes at interfaces through to the development of new materials. A number of techniques are commonly used to study protein adhesion, but few are directly quantitative. Here we describe the use of Nano Orange, a fluorometric assay, to quantitatively assess the adsorption of bovine fibrinogen and albumin onto model hydrophilic (OH terminated) and hydrophobic (CH3 terminated) surfaces. Results obtained using this method allowed the calibration of previously unquantifiable data obtained on the same surfaces using quartz crystal microbalance measurements and an amido black protein assay. Both proteins were found to adsorb with higher affinity but with lower saturation levels onto hydrophobic surfaces. All three analytical techniques showed similar trends in binding strength and relative amounts adsorbed over a range of protein concentrations, although the fluorometric analysis was the only method to give absolute quantities of surface-bound protein. The versatility of the fluorometric assay was also probed by analyzing protein adsorption onto porous superhydrophobic and superhydrophilic surfaces. Results obtained using the assay in conjunction with these surfaces were surface chemistry dependent. Imbibition of water into the superhydrophilic coatings provided greater surface area for protein adsorption, although the protein surface density was less than that found on a comparable flat hydrophilic surface. Superhydrophobic surfaces prevented protein solution penetration. This paper demonstrates the potential of a fluorometric assay to be used as an external calibration for other techniques following protein adsorption processes or as a supplemental method to study protein adsorption. Differences in protein adsorption onto hydrophilic vs superhydrophilic and hydrophobic vs superhydrophobic surfaces are highlighted.

Adsorption↗
PubMed2006

Adsorption of glucose oxidase onto plasma-polymerized film characterized by atomic force microscopy, quartz crystal microbalance, and electrochemical measurement.

Adsorption of glucose oxidase (GOD) onto plasma-polymerized thin films (PPF) with nanoscale thickness was characterized by atomic force microscopy (AFM), quartz crystal microbalance (QCM), and electrochemical measurements. The PPF surface is very flat (less than 1-nm roughness), and its properties (charge and wettability) can be easily changed while retaining the backbone structure. We focused on three types of surfaces: (1) the pristine surface of hexamethyldisiloxane (HMDS) PPF (hydrophobic and neutral surface), (2) an HMDS PPF surface with nitrogen-plasma treatment (hydrophilic and positive-charged surface), and (3) an HMDS PPF surface treated with oxygen plasma (hydrophilic and negative-charged surface). The AFM image showed that the GOD molecules were densely adsorbed onto surface 2 and that individual GOD molecules could be observed. The longer axis of GOD ellipsoid molecules were aligned parallel to the surface, called the "lying position", because of electrostatic association. On surface 1, clusters of GOD molecules did not completely cover the original PPF surface (surface coverage was ca. 60%). The 10-nm-size step height between the GOD clusters and the PPF surface suggests that the longer axes of individual GOD molecules were aligned perpendicular to the surface, called the "standing position". On surface 3, only a few of the GOD molecules were adsorbed because of electrostatic repulsion. These results indicate that the plasma polymerization process can facilitate enhancement or reduction of protein adsorption. The AFM images show a corresponding tendency with the QCM profiles. The QCM data indicate that the adsorption behavior obeys the Langmuir isotherm equation. The amperometric biosensor characteristics of the GOD-adsorbed PPF on a platinum electrode showed an increment in the current because of enzymatic reaction with glucose addition, indicating that enzyme activity was mostly retained in spite of irreversible adsorption.

Adsorption↗
PubMed2004

Multilayers of charged polypeptides as studied by in situ ellipsometry and quartz crystal microbalance with dissipation.

The buildup of poly(L-glutamic acid) (PGA) and poly(L-lysine) (PLL) multilayers on silica and titanium surfaces, with and without an initial layer of polyethyleneimine (PEI), was investigated and characterized by means of in situ ellipsometry and quartz crystal microbalance with dissipation. A two-regime buildup was found in all systems, where the length of the first slow-growing regime is dependent on the structure of the initial layers. In the second fast-growing regime, the film thickness grows linearly while the mass increases more than linearly (close to exponentially) with the number of deposited layers. The film refractive indices as well as the water contents indicate that the film density changes as the multilayer film builds up. The change in film density was proposed to be due to polypeptides diffusing into the multilayer film as they attach. Furthermore, the use of PEI as the initial layer was found to induce a difference in the thickness increments for PGA and PLL.

Electrochemistry↗
PubMed2004

Human immunoglobulin adsorption investigated by means of quartz crystal microbalance dissipation, atomic force microscopy, surface acoustic wave, and surface plasmon resonance techniques.

Time-resolved adsorption behavior of a human immunoglobin G (hIgG) protein on a hydrophobized gold surface is investigated using multitechniques: quartz crystal microbalance/dissipation (QCM-D) technique; combined surface plasmon resonance (SPR) and Love mode surface acoustic wave (SAW) technique; combined QCM-D and atomic force microscopy (AFM) technique. The adsorbed hIgG forms interfacial structures varying in organization from a submonolayer to a multilayer. An "end-on" IgG orientation in the monolayer film, associated with the surface coverage results, does not corroborate with the effective protein thickness determined from SPR/SAW measurements. This inconsistence is interpreted by a deformation effect induced by conformation change. This conformation change is confirmed by QCM-D measurement. Combined SPR/SAW measurements suggest that the adsorbed protein barely contains water after extended contact with the hydrophobic surface. This limited interfacial hydration also contributed to a continuous conformation change in the adsorbed protein layer. The viscoelastic variation associated with interfacial conformation changes induces about 1.5 times overestimation of the mass uptake in the QCM-D measurements. The merit of combined multitechnique measurements is demonstrated.

Adsorption↗
PubMed2005

Analysis of interpenetrating polymer networks via quartz crystal microbalance with dissipation monitoring.

A quartz crystal microbalance with dissipation monitoring (QCM-D) was used to assess the physical properties of interpenetrating polymer networks (IPNs) through swelling experiments in ambient humidity and in phosphate-buffered saline (PBS), pH 7.4. The IPNs, based on acrylamide (AAm) and poly(ethylene glycol) (pEG), swell from thin, rigid films when dry (16.7 +/- 5.2 nm on Si/SiO(2)) to expanded, viscoelastic films when hydrated (107 +/- 24.2 nm on Si/SiO2). The dry IPNs could be analyzed using the Sauerbrey relationship, but for the hydrated films it was necessary to interpret QCM-D data with a Kelvin-Voigt viscoelastic model. A complex modulus |G| of 116 +/- 38.1 kPa for the swollen IPN surface on Si/SiO2 was defined by the model. The QCM-D was also employed to quantify the adsorption of human fibrinogen, a protein important in thrombus formation, onto the IPNs. Fibrinogen adsorption studies demonstrated the sensitivity of the QCM-D, as well as confirmed the nonfouling nature of the IPN surface, where less than 5 ng/cm2 of fibrinogen was adsorbed.

Adsorption↗
PubMed2004

Contact mechanics studies with the quartz crystal microbalance: origins of the contrast factor for polymer gels and solutions.

A contact mechanics methodology utilizing the quartz crystal microbalance (QCM) has been applied to study the spreading behavior of polymer solutions and gels. Changes in the resonant frequency and in the dissipation are monitored as these materials are brought into contact with the electrode surface of the QCM. The primary application is in studies of elastic polymer gels, where spreading over the surface of the QCM is limited by the elasticity of the gel. Simultaneous measurement of the applied loads and displacements, along with measurement of the QCM/gel contact area, the frequency shift, and the dissipation, enable us to calibrate the QCM as a contact sensor. While changes in the frequency and dissipation both depend linearly on the contact area, measurements of the dissipation provide a more reliable indicator. The relationship between the dissipation and the contact area is determined by the solvent viscosity and by the high-frequency intrinsic viscosity of the system of interest. This result is consistent with previous results on the high-frequency rheological behavior of polymer solutions.

Biosensing Techniques↗
PubMed2004

Electrochemical quartz crystal nanobalance study of the adsorption/displacement phenomena of proteins and lipids on Pt.

The electrochemical quartz crystal nanobalance (EQCN) was used to measure the adsorption behavior of a series of lipids (stearate, oleate, linoleate, and gamma-linolenate) on a Pt surface from a phosphate buffer pH 7.0 solution at 295 K and to investigate their adsorption/displacement behavior with the proteins, beta-lactoglobulin and alpha-lactalbumin, which are known to cause fouling during milk processing. The EQCN technique and the complementary technique of cyclic voltammetry measured simultaneously provided information on the efficiency of solubilization of the proteins by these lipids. Excellent agreement was obtained for the surface concentration of adsorbed lipid from the surface charge density from cyclic voltammetry measurements and the change in mass from the EQCN frequency measurements. The Gibbs energy of adsorption showed the lipids to have a strong affinity for the platinum surface. Addition of protein to a preadsorbed lipid layer showed alpha-lactalbumin to be able to coadsorb with the lipids, while beta-lactoglobulin was able to desorb some of the unsaturated lipids but appeared to coadsorb with the saturated lipid, stearate. Addition of lipid to a preadsorbed protein layer showed the unsaturated lipids to be able to displace some of the protein. A comparison of the desorption ability of the lipids showed stearate to be very inefficient at removing protein, while the other three lipids were able to remove each of the proteins, with the order of efficiency for protein desorption being oleate > linoleate > gamma-linolenate.

Adsorption↗
PubMed2005

Hydrogels from a water-soluble zwitterionic polythiophene: dynamics under pH change and biomolecular interactions observed using quartz crystal microbalance with dissipation monitoring.

The water-soluble zwitterionic polythiophene, poly(3-((S)-5-amino-5-carboxyl-3-oxapentyl)-2,5-thiophene) hydrochloride (POWT), is a conjugated polyelectrolyte (CPE) with properties well suited for biochip applications. CPEs readily form hydrogels when exposed to water-based buffer solutions or biomolecule solutions. In this work, we used in situ quartz crystal microbalance with dissipation (QCM-D) monitoring to collect information on the interaction between POWT films exposed to buffers with different pH and POWT/DNA chains. Our data show that POWT swells significantly when exposed to low-pH buffers, such as pH 4 acetate, this is seen as an increase in thickness and decrease in viscosity obtained via a Voight-based modeling of combined f and D QCM-D measurements. The magnitude of thickness and viscosity change upon changing from a pH 10 carbonate buffer to pH 4 acetate is 100% increase in thickness and 50% decrease in viscosity. The response of the hydrogel under pH change is well correlated with fluorescence data from POWT films on glass. The state of the hydrogel is important during interaction with biomolecules; illustrated by the observation that a swollen CPE hydrogel adsorbs a higher amount of DNA than a compacted one. In agreement with previous results, the QCM-D data confirmed that the POWT/DNA hydrogel sense complementary DNA specifically and with negligible binding of noncomplementary DNA. These results are important for efficient constructions of biochips in water environments using this class of materials.

Adsorption↗
PubMed2006

Adsorption kinetics of an engineered gold binding Peptide by surface plasmon resonance spectroscopy and a quartz crystal microbalance.

The adsorption kinetics of an engineered gold binding peptide on gold surface was studied by using both quartz crystal microbalance (QCM) and surface plasmon resonance (SPR) spectroscopy systems. The gold binding peptide was originally selected as a 14-amino acid sequence by cell surface display and then engineered to have a 3-repeat form (3R-GBP1) with improved binding characteristics. Both sets of adsorption data for 3R-GBP1 were fit to Langmuir models to extract kinetics and thermodynamics parameters. In SPR, the adsorption onto the surface shows a biexponential behavior and this is explained as the effect of bimodal surface topology of the polycrystalline gold substrate on 3R-GBP1 binding. Depending on the concentration of the peptide, a preferential adsorption on the surface takes place with different energy levels. The kinetic parameters (e.g., K(eq) approximately 10(7) M(-1)) and the binding energy (approximately -8.0 kcal/mol) are comparable to synthetic-based self-assembled monolayers. The results demonstrate the potential utilization of genetically engineered inorganic surface-specific peptides as molecular substrates due to their binding specificity, stability, and functionality in an aqueous-based environment.

Adsorption↗
PubMed2006

Current rectification with poly-l-lysine-coated quartz nanopipettes.

Ion current rectification with quartz nanopipette electrodes was investigated through the control of the surface charge. The presence and absence of a positively charged poly-l-lysine (PLL) coating resulted in the rectified current with opposite polarity. The results agreed with the theories developed for current-rectifying conical nanopores, suggesting the similar underlying mechanism among asymmetric nanostructure in general. This surface condition dependence can be used as the fundamental principle of multi-purpose real-time in vivo biosensors.

Electric Conductivity↗
PubMed1999

Lysophosphatidylcholine abrogates the CR1 preserving effect of surfactant on quartz-exposed human granulocytes.

The effects of pulmonary surfactant on granulocytes were studied by flow cytofluorometry. Cells from hemolyzed blood were first activated by N-formylmethionyl-leucyl-phenylalanine (fMLP) which mobilizes complement receptor 1 (CR1) from the intracellular pool to the cell surface. The reduced CR1 expression observed after quartz incubation was abolished by a porcine surfactant preparation containing phospholipids and the hydrophobic surfactant proteins. Phospholipids alone had no preservative capacity. However, addition of the surfactant proteins to the phospholipids did not restore the CR1 values to that of intact surfactant, probably due to changed protein structure during the purification procedure. Heating of surfactant at 37 degrees C up to 72 h reduced the preservative effect of surfactant on CR1 expression. Congruent results of CR1 expression were achieved when 1-10% lysophosphatidylcholine was added to the surfactant preparations. Our results imply that lysophosphatidylcholine formed during storage of surfactant at elevated temperatures influences CR1 expression on granulocytes.

Granulocytes↗