Nanocapillary array membranes (NCAMs), comprised of thin (d approximately 5-10 microm) nuclear track-etched polycarbonate sheets containing approximately 10(8) cm(-2) nearly parallel nanometer-diameter capillaries, may act to gate fluid transport between microfluidic channels to effect, for example, sample collection. There is interest in H+-transport across these NCAMs because there is significant practical interest in being able to process analyte-containing samples under different pH conditions in adjacent layers of an integrated microfluidic circuit and because protons, with their inherently high mobility, present a challenge in separating microfluidic environments with different properties. To evaluate the capability of NCAMs to support pH gradients, the proton transport properties of NCAMs were studied using laser scanning confocal fluorescence microscopy (LSCFM). Spatiotemporal maps of [H+] in microfluidic channels adjacent to the NCAMs yield information regarding diffusive and electrokinetic transport of protons. The NCAMs studied here are characterized by a positive zeta potential, zeta > 0, so at small nanocapillary diameters, the overlap of electrical double layers associated with opposite walls of the nanocapillary establish an energy barrier for either diffusion or electrokinetic transport of cations through the nanometer-diameter capillaries due to the positive charge on the nanocapillary surface. Proton transfer through an NCAM into microchannels is reduced for pore diameters, d < or = 50 nm and ionic strengths I < or = 50 mM, while for large pore diameters or solution ionic strengths, the incomplete overlap of electric double layer allows more facile ionic transfer across the membranes. These results establish the operating conditions for the development of multilevel integrated nanofluidic/microfluidic architectures which can support multidimensional chemical analysis of mass-limited samples requiring sequential operations to be implemented at different pH values.
Spherical particles of calcium dioleate were successfully prepared to measure the interaction force of
a calcium dioleate collector colloid at calcite and fluorite surfaces. Scanning electron microscopy (SEM),
atomic force microscopy (AFM), Fourier transform infrared (FTIR) spectroscopy, and electrophoretic mobility
measurements were used to characterize the specially prepared calcium dioleate spheres. FTIR spectra
show that the spheres have the same spectral properties as untreated (freshly precipitated) calcium dioleate.
SEM imaging of the sphere surface and AFM roughness measurements indicate that these spheres can
be used as colloidal probes for interaction force measurements. AFM interaction force measurements
between calcium dioleate spheres and mineral surfaces were conducted at selected pH values from pH 5.2
to pH 10.0. The attractive force and adhesion force between the calcium dioleate sphere and the fluorite
surface were found to be much stronger and longer-range than those measured between the calcium
dioleate sphere and the calcite surface. The range and magnitude of these attractive forces were found
to be pH dependent in the case of fluorite. These results are discussed in conjunction with streaming
potential measurements, contact angle measurements, and the flotation behavior of calcite and fluorite
with oleate as the collector.
Streaming potential measurements provide valuable information for the validation and interpretation of interfacial phenomena that occur at flat macroscopic surfaces. Planar substrates have been extensively used for the interpretation of events, which occur at particulate surfaces; however, these flat surfaces are often only questionably representative of their particulate counterparts due to variations in surface chemistry and topography. In this study, the zeta potential from planar macroscopic surfaces of PMMA, mica, graphite, fluorite, and calcite have been calculated from streaming potentials measured in aqueous solutions using an asymmetric clamping cell. These zeta potentials have been found to significantly contribute to understanding and interpretation of interfacial phenomena influenced by Coulombic interactions including adsorption, surface forces, and the structure of surface micelles.
Spherical calcium dioleate particles ( approximately 10 mum in diameter) were used as AFM (atomic force microscope) probes to measure interaction forces of the collector colloid with calcite and fluorite surfaces. The attractive AFM force between the calcium dioleate sphere and the fluorite surface is strong and has a longer range than the DLVO (Derjaguin-Landau-Verwey-Overbeek) prediction. The AFM force between the calcium dioleate sphere and the mineral surfaces does not agree with the DLVO prediction. Consideration of non-DLVO forces, including the attractive hydrophobic force and the repulsive hydration force, was necessary to explain the experimental results. The non-DLVO interactions considered were justified by the different interfacial water structures at calcite- and fluorite-water interfaces as revealed by the numerical computation experiments with molecular dynamics simulation.
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