Biomedical subjects

Costas Tsouris

Publications and source records attributed to Costas Tsouris.

12 recordsLinked to original sources

PubMed2006

Electrostatic surface interactions in mixtures of symmetric and asymmetric electrolytes: a Monte Carlo study.

Canonical Monte Carlo simulations of the interaction between a uniformly charged spherical particle and a discretely charged planar surface in solutions of symmetric and asymmetric electrolytes were performed. To assess the nature of the interactions, the force exerted on the colloidal particle perpendicular to the planar surface was calculated. Attractive minima in the interaction force between the similarly charged surfaces reveal the occurrence of two phenomena: long-range attraction of electrostatic origin and short-range attraction due to depletion effects. The degree of electrostatic coupling determines the magnitude and range of like-charge attraction between the two surfaces.

Journal Article↗

PubMed2006

Electrosorption capacitance of nanostructured carbon-based materials.

The fundamental mechanism of electrosorption of ions developing a double layer inside nanopores was studied via a combination of experimental and theoretical studies. A novel graphitized-carbon monolithic material has proven to be a good electrical double-layer capacitor that can be applied in the separation of ions from aqueous solutions. An extended electrical double-layer model indicated that the pore size distribution plays a key role in determining the double-layer capacitance in an electrosorption process. Because of the occurrence of double-layer overlapping in narrow pores, mesopores and micropores make significantly different contributions to the double-layer capacitance. Mesopores show good electrochemical accessibility. Micropores present a slow mass transfer of ions and a considerable loss of double-layer capacitance, associated with a shallow potential distribution inside pores. The formation of the diffuse layer inside the micropores determines the magnitude of the double-layer capacitance at low electrolyte concentrations and at conditions close to the point of zero charge of the material. The effect of the double-layer overlapping on the electrosorption capacitance can be reduced by increasing the pore size, electrolyte concentration, and applied potential. The results are relevant to water deionization.

Adsorption↗

PubMed2005

Field studies on the formation of sinking CO2 particles for ocean carbon sequestration: effects of injector geometry on particle density and dissolution rate and model simulation of plume behavior.

We have carried out the second phase of field studies to determine the effectiveness of a coflow injector which mixes liquid CO2 and ambient seawater to produce a hydrate slurry as a possible CO2 delivery method for ocean carbon sequestration. The experiments were carried out at ocean depths of 1000-1300 m in Monterey Bay, CA, using a larger injector than that initially employed under remotely operated vehicle control and imaging of the product. Solidlike composite particles comprised of water, solid CO2 hydrate, and liquid CO2 were produced in both studies. In the recent injections, the particles consistently sank at rates of approximately 5 cm s(-1). The density of the sinking particles suggested that approximately 40% of the injected CO2 was converted to hydrate, while image analysis of the particle shrinking rate indicated a CO2 dissolution rate of 0.76-1.29 micromol cm(-2) s(-1). Plume modeling of the hydrate composite particles suggests that while discrete particles may sink 10-70 m, injections with CO2 mass fluxes of 1-1000 kg s(-1) would result in sinking plumes 120-1000 m belowthe injection point.

Carbon↗

PubMed2005

Surface charge heterogeneities measured by atomic force microscopy.

Unfavorable aggregation and deposition of colloidal particles in natural and engineered systems is still a subject of debate. Complicating factors such as surface roughness, secondary minimum aggregation, and the nature of discrete surface charge and surface potential make it difficult to attribute a specific cause to these phenomena. The presence of surface charge heterogeneity and its influence on interaction forces, which are responsible for aggregation and deposition, are studied in this work through the application of atomic force microscopy (AFM). Force-volume-mode AFM was used to map interaction forces on a surface and relate them to surface charge heterogeneities. The experimental system consisted of a silica plate and a standard silicon nitride AFM tip. Copper ions were used for sorption on the silica surface in order to modify the surface charge and cause charge reversal. Different concentrations of copper ions were selected to identify conditions of partial coverage of the silica surface. The pH and ionic strength of the solutions were varied, and the extension of the surface charge modification and its influence on the resulting interaction forces were monitored via AFM force measurements. Depending on the pH and ionic strength, the interaction force was found to change at certain regions on the surface from attraction to either weak or strong repulsion. Force imaging allowed the visual localization of zones of strong repulsive interaction that diminished in size with increasing ionic strength. X-ray photoelectron spectroscopy analysis was used to confirm the presence of copper on the surface. Local charge differences on a surface result in local differences in surface forces, not only in magnitude but also in direction. This behavior may explain the aggregation, deposition, and transport of colloidal particles under unfavorable chemical conditions.

Colloids↗

PubMed2005

Behavior of mixtures of symmetric and asymmetric electrolytes near discretely charged planar surfaces: a Monte Carlo study.

Canonical Monte Carlo (CMC) simulations are employed in this work in order to study the structure of the electrical double layer (EDL) near discretely charged planar surfaces in the presence of symmetric and asymmetric indifferent electrolytes within the framework of a primitive model. The effects of discreteness and strength of surface charge, charge asymmetry, and size asymmetry are specific focuses of this work. The CMC simulation protocol is initially tested against the classical theory, the modified Gouy-Chapman (GC) theory, in order to assess the reliability of the simulation results. The CMC simulation results and the predictions of the classical theory show good agreement for 1:1 electrolytes and low surface charge, at which conditions the GC theory is valid. Simulations with symmetric and asymmetric electrolytes and mixtures of the two demonstrate that size plays an important role in determining the species present in the EDL and how the surface charge is screened. A size-exclusion effect could be consistently detected. Although it is energetically favorable that higher-valence ions screen the surface charge, their larger size prevents them from getting close to the surface. Smaller ions with lower valences perform the screening of the charge, resulting in higher local concentrations of small ions close to the surface. The simulations also showed that the strength of the surface charge enhances the size-exclusion effect. This effect will definitely affect the magnitude of the forces between interacting charged surfaces.

Journal Article↗

PubMed2004

Hydrate composite particles for ocean carbon sequestration: field verification.

This paper reports on the formation and dissolution of CO2/seawater/CO2 hydrate composite particles produced during field experiments in Monterey Bay, CA using a CO2 injector system previously developed in the laboratory. The injector consisted of a coflow reactor wherein water was introduced as a jet into liquid CO2, causing vigorous mixing of the two immiscible fluids to promote the formation of CO2 hydrate that is stable at ambient pressures and temperatures typical of ocean depths greater than approximately 500 m. Using flow rate ratios of water and CO2 of 1:1 and 5:1, particulate composites of CO2 hydrate/liquid CO2/seawater phases were produced in seawater at depths between 1100 and 1300 m. The resultant composite particles were tracked by a remotely operated vehicle system as they freely traveled in an imaging box that had no bottom or top walls. Results from the field experiments were consistent with laboratory experiments, which were conducted in a 70 L high-pressure vessel to simulate the conditions in the ocean at intermediate depths. The particle velocity and volume histories were monitored and used to calculate the conversion of CO2 into hydrate and its subsequent dissolution rate after release into the ocean. The dissolution rate of the composite particles was found to be higher than that reported for pure CO2 droplets. However, when the rate was corrected to correspond to pure CO2, the difference was very small. Results indicate that a higher conversion of liquid CO2 to CO2 hydrate is needed to form negatively buoyant particles in seawater when compared to freshwater, due primarily to the increased density of the liquid phase but also due to processes involving brine rejection during hydrate formation.

Atmospheric Pressure↗

PubMed2004

Kinetics of soil ozonation: an experimental and numerical investigation.

This study investigates the use of ozone for soil remediation. Batch experiments, in which ozone-containing gas was continuously recycled through a soil bed, were conducted to quantify the rate of ozone self-decomposition and the rates of ozone interaction with soil organic and inorganic matter. Column experiments were conducted to measure ozone breakthrough from a soil column. Parameters such as ozone flow rate, soil mass, and ozonation time were varied in these experiments. After ozone concentration had reached steady state, the total organic carbon concentration was measured for all soil samples. The ozonation efficiency, represented by the ratio of soil organic matter consumed to the total ozone input, was quantified for each experiment. Numerical simulations were conducted to simulate experimentally obtained column breakthrough curves. Experimentally obtained kinetic rate constants were used in these simulations, and the results were in good agreement with experimental data. In contrast to previous studies in which soil inorganic matter was completely ignored, our experiments indicate that soil inorganic matter may also promote depletion of ozone, thus reducing the overall ozonation efficiency. Three-dimensional numerical simulations were conducted to predict the efficacy of ozonation for soil remediation in the field. These simulations indicate that such ozonation can be very effective, provided that effective circulation of ozone is achieved through appropriately placed wells.

Bioreactors↗

PubMed2003

Copper uptake by silica and iron oxide under high surface coverage conditions: surface charge and sorption equilibrium modeling.

A sorption modeling approach based on surface complexation concepts was applied to predict copper uptake and its effects on the surface electrostatic potential of ferric oxide and silica colloids. Equilibrium modeling of copper uptake by ferric oxide using the traditional surface complexation model (SCM) was reasonably successful with some discrepancies especially in the acidic pH ranges and high colloid concentration cases. Good predictions of the ferric oxide charge reversals during uptake were obtained from the modeling. Based on the SCM predictions, copper removal from solution is due to the outer-sphere complexation of the first hydrolysis product, resulting in the surface-metal complex SO(-)CuOH(+). The SCM was found to be insufficient to describe copper uptake by silica particles. To address discrepancies between experimental data and SCM predictions, the SCM was modified to include attributes of the surface polymer model (SPM), which incorporates sorption of the dimeric copper species Cu(2)(OH)(2)(2+). The continuum model (CM) was also studied as a second modification to the SCM to include formation of surface precipitates. Both the SPM and the CM were successful in modeling copper uptake and zeta potential variations as a function of pH at various solution conditions and colloid concentrations. From the SPM and CM predictions, it was concluded that for systems with high surface loadings, copper removal from solution occurs due to the formation of both monomeric and dimeric surface complexes, as well as through precipitation mechanisms.

Journal Article↗

PubMed2003

CO2 hydrate composite for ocean carbon sequestration.

Rapid CO2 hydrate formation was investigated with the objective of producing a negatively buoyant CO2-seawater mixture under high-pressure and low-temperature conditions, simulating direct CO2 injection at intermediate ocean depths of 1.0-1.3 km. A coflow reactor was developed to maximize CO2 hydrate production by injecting water droplets (e.g., approximately 267 microm average diameter) from a capillary tube into liquid CO2. The droplets were injected in the mixing zone of the reactor where CO2 hydrate formed at the surface of the water droplets. The water-encased hydrate particles aggregated in the liquid CO2, producing a paste-like composite containing CO2 hydrate, liquid CO2, and water phases. This composite was extruded into ambient water from the coflow reactor as a coherent cylindrical mass, approximately 6 mm in diameter, which broke into pieces 5-10 cm long. Both modeling and experiments demonstrated that conversion from liquid CO2 to CO2 hydrate increased with water flow rate, ambient pressure, and residence time and decreased with CO2 flow rate. Increased mixing intensity, as expressed by the Reynolds number, enhanced the mass transfer and increased the conversion of liquid CO2 into CO2 hydrate. Using a plume model, we show that hydrate composite particles (for a CO2 loading of 1000 kg/s and 0.25 hydrate conversion) will dissolve and sink through a total depth of 350 m. This suggests significantly better CO2 dispersal and potentially reduced environmental impacts than would be possible by simply discharging positively buoyant liquid CO2 droplets. Further studies are needed to address hydrate conversion efficiency, scale-up criteria, sequestration longevity, and impact on the ocean biota before in-situ production of sinking CO2 hydrate composite can be applied to oceanic CO2 storage and sequestration.

Carbon Dioxide↗

PubMed2003

Brownian motion in confinement.

This research modifies an earlier approach based on the single-wall reflection method to predict the perpendicular and parallel diffusion coefficients of a Brownian sphere in confinement. The modified version provides predictions that match experimental data reported in the literature more accurately than those provided by other available models, including the linear superposition approximation, the coherent superposition approximation, and Oseen's equation.

Journal Article↗

PubMed2002

Electrosorption of ions from aqueous solutions by nanostructured carbon aerogel.

Electrosorption is generally defined as potential-induced adsorption on the surface of charged electrodes. After polarization of the electrodes, ions are removed from the electrolyte solution by the imposed electric field and adsorbed onto the surface of the electrodes. Experimental and modeling studies were conducted using two types of carbon aerogel composites of different surface areas to provide a better understanding on the mechanisms of electrosorption. The experimental results revealed that no significant specific adsorption of F- ions occurred, while strong specific adsorption was observed for NO3- and Cu2+ ions. In addition, although the two types of carbon aerogel electrodes had different surface areas, their capacities were found to be very similar because of the electrical double-layer overlapping effect in micropores. An electrical double-layer model developed in our previous work (16), in which the electrical double-layer overlapping correction is included, is expanded in the present work by considering the effect of the specific adsorption on the electrosorption process. Modeling results were compared with experimental data obtained under various conditions. When the overlapping effect and specific adsorption were considered, the model provided results that were in good agreement with experimental data.

Journal Article↗

PubMed2002

Influence of metal ion sorption on colloidal surface forces measured by atomic force microscopy.

Atomic force microscopy (AFM) is employed to directly measure colloidal surface forces between a silica particle and a smooth glass plate in an aqueous solution with or without the presence of copper ions. Without the presence of copper ions, results show that the force between these two surfaces is repulsive and that its magnitude decreases with increasing ionic strength and decreasing pH. The surface forces are calculated based on the Derjaguin-Landau-Verwey-Overbeek (DLVO) theory for constant surface charge and are then compared with AFM force measurements. A good agreement between theory and experimental data is reported except at very small separation distances (<3 nm) between the silica particle and the glass plate. This behavior may be attributed to non-DLVO forces, such as the hydration effect that results from the bounded water molecules on the surface of the silica particle, or to surface roughness. When copper ions are present in acidic aqueous solutions, the magnitude of the force is found to be the same as that without the presence of copper ions, which indicates that no sorption of copper ions by the silica particle occurs under these conditions. Near neutral pH, sorption of copper ions causes charge reversal for the silica particle from negative to positive. Therefore, the force between the silica particle and the glass plate changes from repulsive to attractive. The transient zeta-potential of the silica particle during sorption of copper ions is determined by representing the experimental data with the DLVO theory. In alkaline solutions, where removal of copper ions is known to occur mainly by bulk precipitation, the measured force is similar to that without the presence of copper ions, which suggests that sorption does not occur under such conditions.

Colloids↗