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PubMed2002

Influence of ionic strength and cation charge on transport of colloidal particles in fractured shale saprolite.

The role of solution chemistry (cation charge and concentration) and particle size on colloid transport was examined in an intact monolith of fractured shale saprolite (highly weathered rock). Recovery of the microsphere tracers consistently decreased with increasing ionic strength of either mono- (Na+) or divalent- (Ca2+) dominated solutions, but a much greater concentration of Na+ in the influent solution was required to result in a similar reduction in colloid recovery as compared to Ca2+. However, composition of the solution along the flow path, and hence the degree of microsphere retention, was also strongly influenced by cation exchange and diffusive exchange between pore water in the fractures and in the fine-grained, Ca- and Mg-rich matrix. The influence of "matrix diffusion" on solute transport is also evident in the 5-fold difference between the arrival of the center-of-mass of microspheres as compared to the much later arrival of a bromide tracer. Particle size affected the extent of microsphere transport, but the solution chemistry appears to be a more dominant control. While confirming the importance of ionic strength, counterion charge, and particle size on colloid migration, this study emphasizes the profound effect that pore structure and geochemical processes such as cation exchange have on solution chemistry and thus on colloid transport.

Cations, Divalent↗
PubMed2003

Forces between colloid particles in natural waters.

The origin and nature of interparticle forces acting on colloid surfaces in natural waters has been examined using an atomic force microscope. Natural colloids were represented by a surface film of iron oxide precipitated onto spherical SiO2 particles, and the effects of adsorbed natural organic matter (NOM), solution pH, and ionic composition on the force-separation curves were investigated. NOM from both riverine and marine environments was strongly adsorbed to the iron oxide surface. Under conditions of low ionic strength, the interparticle forces were dominated by electrostatic repulsion arising from negative functional groups on the NOM, except at very small separations (<10 nm) where repulsive forces arising from steric interference of the NOM molecules were also present. At high ionic strength (e.g., seawater) or low pH, the electrostatic forces were largely absent, allowing steric repulsion forces to dominate. In addition, adhesive bridging between surfaces by adsorbed NOM was observed, creating a strong energy barrier to spontaneous disaggregation of colloid aggregates. Our results demonstrate that adsorbed NOM dominates the surface forces and thus stability with respect to aggregation of natural water colloids.

Adsorption↗
PubMed2004

Colloid formation at waste plume fronts.

Highly saline and caustic tank waste solutions containing radionuclides and toxic metals have leaked into sediments at U.S. Department of Energy (DOE) facilities such as the Hanford Site (Washington state). Colloid transport is frequently invoked to explain migration of radionuclides and metals in the subsurface. To understand colloid formation during interactions between highly reactive fluids and sediments and its impact on contaminant transport, we simulated tank waste solution (TWS) leakage processes in laboratory columns at ambient and elevated (70 degrees C) temperatures. We found that maximum formation of mobile colloids occurred at the plume fronts (hundreds to thousands times higher than within the plume bodies or during later leaching). Concentrations of suspended solids were as high as 3 mass %, and their particle sizes ranged from tens of nanometers to a few micrometers. Calcium carbonate is always one of the dominant phases of the plume front colloids, while the other phases varied with solution pH and temperature. During infiltration of the leaked high-Na+ waste solution, rapid and completed Na+ replacement of exchangeable Ca2+ and Mg2+ from the sediment caused accumulation of these divalent cations at the moving plume front. Precipitation of supersaturated Ca2+/Mg2+-bearing minerals caused dramatic pH reduction atthe plume front. In turn, the reduced pH caused precipitation of other minerals. This understanding can help predict the behavior of contaminant trace elements carried by the tank waste solutions and could not have been obtained through conventional batch studies.

Adsorption↗
PubMed2006

Size fractionation and characterisation of fresh water colloids and particles: split-flow thin-cell and electron microscopy analyses.

Split-flow thin-cell (SPLITT) was employed in conventional mode (CSF), to size-fractionate colloids and particles from a selected freshwater. Imaging and quantification by calculations of particle size distributions (PSDs) and shape factors were performed on sample analyzed by conventional high vacuum scanning electron microscopy (SEM) and environmental SEM (ESEM), to investigate the ability of SPLITT to make accurate and nonperturbing separations. SEM and ESEM images of unperturbed and SPLITT-generated fractions were used in order to obtain qualitative and quantitative information about the properties of colloids and particles. Particle size distributions (PSDs) showed that separations were very good, agreeing with theoretical behavior. ESEM PSDs showed that up to 87-88% of the material in the a fraction (expected to be <1 microm) was in fact less than 1 microm and in the b fraction (>1 microm) 87-95% of the material was the expected size. The SEM data indicated a slightly higher contamination of the b fraction with the presence of submicron colloids. Moreover, analysis of conformations indicated significant nonsphericity in unfractionated colloids and particles, but after SPLITT fractionation, shape factors showed that particles were significantly more spherical than before separation.

Chemical Fractionation↗
PubMed2005

Light-regulated electrostatic interactions in colloidal suspensions.

The net charge of a colloidal particle was controlled using light and a new photocleavable self-assembled monolayer (SAM). The SAM contained a terminal ammonium group and a centrally located carboxylic acid group that was masked with an ortho-nitrobenzyl functionality. Once exposed to UV light, the 2-nitrobenzyl group was cleaved, therefore transforming the colloidal particle from a net positive (silica-SAM-NH3+) to a net negative (silica-SAM-COO-) charge. By varying the UV exposure time, their zeta potential could be tailored between +26 and -60 mV at neutral pH. To demonstrate a photoinduced gel-to-fluid phase transition, a binary colloidal suspension composed of silica-SAM-NH3+ and negatively charged, rhodamine-labeled silica particles was mixed to form a gel. Exposure to UV light rendered all of the particles negative and therefore converted the system into a colloidal fluid that settles to form a dense sediment.

Colloids↗
PubMed2005

Self-assembly of active IrO2 colloid catalyst on an ITO electrode for efficient electrochemical water oxidation.

Active catalysts for water oxidation to evolve O(2) are required for the construction of artificial photosynthetic devices that are expected to be promising energy-providing systems in the future. The citrate-stabilized IrO(2) colloid was self-assembled onto an indium tin oxide (ITO) electrode to form a monolayer of the colloidal IrO(2) particles when it was dipped in the colloid solution. The self-assembly could be achieved by a chemical interaction between carboxylate groups on the citrate stabilizer and hydroxyl groups on the ITO surface to form ester bonds. Efficient electrocatalysis for water oxidation was demonstrated using the electrode modified by the self-assembled IrO(2) colloid to yield the highest turnover frequency ((2.3-2.5) x 10(4) h(-1)) of IrO(2) in the hitherto-reported catalysts for electrochemical water oxidation.

Catalysis↗
PubMed1996

Comparative in vitro evaluation of several colloidal systems, nanoparticles, nanocapsules, and nanoemulsions, as ocular drug carriers.

Three different colloidal carriers, namely, nanoparticles and nanocapsules made of poly-epsilon-caprolactone and submicron emulsions, were designed, and their capacity for increasing the comeal penetration of drugs was investigated. The three systems differed in their inner structure and composition, but they had a similar size (200-250 nm) and a negative superficial charge (-16 to -42 mV). Indomethacin, which was used as a model drug, was dispersed at a molecular level within the colloidal systems, no chemical interaction between the polymer and the drug being detected. Release of the encapsulated indomethacin occurred very rapidly upon high dilution in a buffered medium and was independent of the composition of the system. The in vitro comeal penetration of the encapsulated indomethacin was more than 3-fold that of the commercial eye drops. This increased penetration was similar for the three formulations investigated, which therefore excludes the influence of the inner structure or chemical composition of the colloidal systems on the comeal penetration of indomethacin. Thus, it could be stated that the main factor responsible for the favorable comeal transport of indomethacin is the colloidal nature of these carriers rather than their inner structure or composition.

Animals↗
PubMed2004

Rheology of binary colloidal structures assembled via specific biological cross-linking.

The selectivity and range of energies offered by specific biological interactions serve as valuable tools for engineering the assembly of colloidal particles into novel materials. In this investigation, high affinity biological interactions between biotin-coated "A" particles (RA = 0.475 microm) and streptavidin-coated "B" particles (RB = 2.75 microm) drive the self-assembly of a series of binary colloidal structures, from colloidal micelles (a large B particle coated by smaller A particles) to elongated chain microstructures (alternating A and B particles), as the relative number of small (A) to large (B) particles (2 < or = NA/NB < or = 200) is decreased at a low total volume fraction (10(-4) < or = phiT < or = 10(-3)). At a significantly higher total volume fraction (phiT > or = 10(-1)) and a low number ratio (NA/NB = 2), the rheological behavior of volume-filling particle networks connected by streptavidin-biotin bonds is characterized. The apparent viscosity (eta) as a function of the shear rate gamma, measured for networks at phiT = 0.1 and 0.2, exhibits shear-rate-dependent flow behavior, and both the apparent viscosity and the extent of shear thinning increase upon an increase of a factor of 2 in the total volume fraction. Micrographs taken before and after shearing show a structural breakdown of the flocculated binary particle network into smaller flocs, and ultimately a fluidlike suspension, with increasing shear rate. Rheological measurements provide further proof that suspension microstructure is governed by specific biomolecular interactions, as control experiments in which the streptavidin molecules on particles were blocked displayed Newtonian flow behavior. This investigation represents the first attempt at measuring the rheology of colloidal suspensions where assembly is driven by biomolecular cross-linking.

Biotin↗
PubMed2004

Parameters influencing the templated growth of colloidal crystals on chemically patterned surfaces.

The influence of various experimental parameters on the vertical deposition and structure formation of colloidal crystals on chemically patterned surfaces, with hydrophilic and hydrophobic areas, was investigated. The pattern dimensions range from about 4 to 400 microm, which is much larger than the individual particle size (255 nm), to control the microscopic crystal shape rather than influencing the crystal lattice geometry (as achieved in colloidal epitaxy). The deposition resolution and selectivity were tested by varying the particle concentration in the suspension, the substrate withdrawing speed, pattern size and orientation, and wetting contrast between the hydrophilic and hydrophobic regions. The evolution of colloidal crystal thickness with respect to the pattern dimensions and deposition parameters was further studied. Our results show that the pattern size has a rather strong influence on the deposited number of colloid layers and on the crystal quality. Better results are obtained when the lines of a stripe pattern are oriented parallel to the withdrawing direction rather than perpendicular. The deposition resolution (defined as the minimum feature size on which particles can be deposited) depends on the wetting contrast and increases with lower average hydrophobicity of the substrate.

Colloids↗
PubMed2004

Bioinert solution-cross-linked hydrogen-bonded multilayers on colloidal particles.

Bioinert polyelectrolyte multilayers comprised of poly(acrylic acid) and polyacrylamide were deposited on colloidal particles (1.7 microm in diameter) at low pH conditions by layer-by-layer assembly using hydrogen-bonding interactions. The multilayer films were coated uniformly on the colloidal particles without causing any flocculation of the colloids, and the deposited films were subsequently cross-linked by a single treatment of a carbodiimide aqueous solution. The lightly cross-linked multilayer films show excellent stability at physiological conditions (pH 7.4, phosphate-buffered saline), whereas untreated multilayer films dissolved. The multilayer-coated surfaces, both on flat substrates and on colloidal particles, exhibit excellent resistance toward mammalian cell adhesion. With this new solution-based cross-linking method, bioinert H-bonded multilayer coatings offer potential for biomedical applications.

Acrylic Resins↗
PubMed2004

Thin film interference of colloidal thin films.

A stairlike colloidal crystal thin film composed of poly(styrene-methyl methacrylate-acrylic acid) (P(St-MMA-AA)) monodispersed colloids was fabricated on an inclined silicon substrate. Different bright colors were observed on the various parts of the film with different layers as white light irradiated perpendicularly on it. The relationship between the colors and layers of the film was investigated and discussed according to the principle of thin film interference. On the basis of the phenomenon of thin film interference, a one-layer colloidal film having uniform color was researched and it would display diverse colors before and after swollen by styrene (St). A circular stairlike colloidal film was achieved to mimic the colors of the peacock tail feather.

Acrylates↗
PubMed2005

Connected open structures from close-packed colloidal crystals by hyperthermal neutral beam etching.

We report the fabrication of connected open structures from close-packed colloidal crystals by hyperthermal neutral beam etching. Colloidal crystal films of polystyrene microspheres were prepared by a vertical deposition method. Exposure of the colloidal crystal films to hyperthermal neutral beam made isolated microspheres in the face-centered cubic lattice, each of which was connected with its twelve nearest neighbors through very thin cylinders. Due to the charge neutrality of impinging gas molecules of the hyperthermal neutral beam, the spherical shape of polymer microspheres was almost maintained during the etching process. The Bragg reflection peaks were modulated by the etched volume of colloidal crystals. Finally, the inverse structures of such open structures were replicated by a simple room-temperature chemical vapor deposition and subsequently burning out polymer template spheres.

Colloids↗
PubMed2006

Interaction forces measured using AFM between colloids and surfaces coated with both dextran and protein.

Both proteins and polysaccharides are biopolymers present on a bacterial surface that can simultaneously affect bacterial adhesion. To better understand how the combined presence of proteins and polysaccharides might influence bacterial attachment, adhesion forces were examined using atomic force microscopy (AFM) between colloids (COOH- or protein-coated) and polymer-coated surfaces (BSA, lysozyme, dextran, BSA+dextran and lysozyme+dextran) as a function of residence time and ionic strength. Protein and dextran were competitively covalently bonded onto glass surfaces, forming a coating that was 22-33% protein and 68-77% dextran. Topographic and phase images of polymer-coated surfaces obtained with tapping mode AFM indicated that proteins at short residence times (<1 s) were shielded by dextran. Adhesion forces measured between colloid and polymer-coated surfaces at short residence times increased in the order protein+dextran < or = protein < dextran. However, the adhesion forces for protein+dextran-coated surface substantially increased with longer residence times, producing the largest adhesion forces between polymer coated surfaces and the colloid over the longest residence times (50-100 s). It was speculated that with longer interaction times the proteins extended out from beneath the dextran and interacted with the colloid, leading to a molecular rearrangement that increased the overall adhesion force. These results show the importance of examining the effect of the combined adhesion force with two different types of biopolymers present and how the time of interaction affects the magnitude of the force obtained with two-polymer-coated surfaces.

Colloids↗
PubMed2006

Fabrication of colloidal doublets by a salting out-quenching-fusing technique.

It is well-known that high ionic strength promotes colloid aggregation. Here we show that, by controlling this aggregation process, we can produce high yields of homodoublet and heterodoublet polymer colloids. The aggregation process is started by increasing the ionic strength to roughly 250 mM KCl. After approximately the rapid flocculation time, we quench the "reaction" by mixing in a large quantity of deionized water, which dilutes the ionic strength and prevents further aggregation. At this point, the suspension consists primarily of singlet and doublet particles. Through heating above the glass transition temperature of the polymers, the doublets are fused together and remain intact even after sonication. It is also shown that heterodoublets can include a silica particle together with a polymer colloid. The salting out-quenching-fusing technique is a rapid, easy-to-perform, repeatable process for fabricating colloidal doublets from polymers and other materials.

Amidines↗
PubMed2005

Combined optical tweezers/ion beam technique to tune colloidal masks for nanolithography.

A method is presented to control the in-plane ordering, size, and interparticle distance of nanoparticles fabricated by evaporation through a mask of colloidal particles. The use of optical tweezers combined with critical point drying gives single-particle position control over the colloidal particles in the mask. This extends the geometry of the colloidal masks from (self-organized) hexagonal to any desired symmetry and spacing. Control over the mask's hole size is achieved by MeV ion irradiation, which causes the colloids to expand in the in-plane direction, thus shrinking the size of the holes. After modification of the mask, evaporation at different angles with respect to the mask gives additional control over structure and interparticle distance, allowing nanoparticles of different materials to be deposited next to each other. We demonstrate large arrays of metal nanoparticles with dimensions in the 15-30 nm range, with control over the interparticle distance and in-plane ordering.

Colloids↗
PubMed2004

Equilibrium cluster formation in concentrated protein solutions and colloids.

Controlling interparticle interactions, aggregation and cluster formation is of central importance in a number of areas, ranging from cluster formation in various disease processes to protein crystallography and the production of photonic crystals. Recent developments in the description of the interaction of colloidal particles with short-range attractive potentials have led to interesting findings including metastable liquid-liquid phase separation and the formation of dynamically arrested states (such as the existence of attractive and repulsive glasses, and transient gels). The emerging glass paradigm has been successfully applied to complex soft-matter systems, such as colloid-polymer systems and concentrated protein solutions. However, intriguing problems like the frequent occurrence of cluster phases remain. Here we report small-angle scattering and confocal microscopy investigations of two model systems: protein solutions and colloid-polymer mixtures. We demonstrate that in both systems, a combination of short-range attraction and long-range repulsion results in the formation of small equilibrium clusters. We discuss the relevance of this finding for nucleation processes during protein crystallization, protein or DNA self-assembly and the previously observed formation of cluster and gel phases in colloidal suspensions.

Colloids↗
PubMed2005

Controlled assembly of jammed colloidal shells on fluid droplets.

Assembly of colloidal particles on fluid interfaces is a promising technique for synthesizing two-dimensional microcrystalline materials useful in fields as diverse as biomedicine, materials science, mineral flotation and food processing. Current approaches rely on bulk emulsification methods, require further chemical and thermal treatments, and are restrictive with respect to the materials used. The development of methods that exploit the great potential of interfacial assembly for producing tailored materials have been hampered by the lack of understanding of the assembly process. Here we report a microfluidic method that allows direct visualization and understanding of the dynamics of colloidal crystal growth on curved interfaces. The crystals are periodically ejected to form stable jammed shells, which we refer to as colloidal armour. We propose that the energetic barriers to interfacial crystal growth and organization can be overcome by targeted delivery of colloidal particles through hydrodynamic flows. Our method allows an unprecedented degree of control over armour composition, size and stability.

Coated Materials, Biocompatible↗
PubMed1977

The pinocytosis of 125I-labelled poly(vinylpyrrolidone), [14C]sucrose and colloidal [198Au]gold by rat yolk sac cultured in vitro.

The rates of uptake of 125I-labelled poly(vinylpyrrolidone), [14C]sucrose and colloidal [198Au]gold by 17.5-day rat yolk sac cultured in vitro were studied. Over a 6.5h period each substrate was accumulated at a constant and reproducible rate of approx. 2microliter/h per mg of protein. After accumulation in vitro, the three substances were released from the tissue into substrate-free medium at low rates. Sucrose present in the medium at concentrations up to 10 mg/ml was without effect on the accumulation of either [14C]sucrose or 125I-labelled poly(vinylpyrrolidone), but at higher concentrations inhibited the uptake of both substrates. Some batches of colloidal [198Au]gold had a significantly higher Endocytic Index (up to 5 microliter/h per mg of protein). The Endocytic Index of such a batch decreased with increasing substrate concentration, but colloidal gold did not decrease the Endocytic Index of 125I-labelled poly(vinylpyrrolidone). It is concluded that the three substrates enter the yolk sac by pinocytosis in the liquid phase. Those batches of colloidal [198Au]gold with higher Endocytic Indices are considered to enter also by adsorption on membrane binding-sites.

Animals↗