PubMed · 12380801
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Catherine J Murphy. 2002-10-01. Optical sensing with quantum dots.. https://doi.org/10.1021/ac022124v
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A simple modified Poisson-Boltzmann formalism, which accounts also for those interactions between electrolyte ions and colloidal particles not included in the mean potential, is used to calculate the force between two parallel plates. It is shown that the short-range interactions between ions and plates, such as those due to the change in the hydration free energy of a structure-making/breaking ion that approaches the interface, affect the double layer interaction at large separations through the modification of the surface potential and surface charge density. While at short separations (below the range of the short-range ion-hydration forces) the interaction can be attractive, at larger separations the interaction is always repulsive, as in the traditional theory. When the long-range van der Waals interactions between the ions and the system (ion-dispersion interactions) are accounted for in the modified Poisson-Boltzmann approach, an attractive force between plates can be generated. At sufficiently large separations, this attraction can become even stronger than the traditional van der Waals attraction between plates of finite thickness, thus generating a dominant long-range 'double layer attraction'. At small plate separations, the attraction generated by the ion-dispersion forces combined with the electrostatic repulsion due to the double layers overlap can lead to a variety of interactions, from a weak attraction (which is typically by at least one order of magnitude smaller than the traditional van der Waals attraction between plates) to a strong double layer repulsion (for sufficiently large surface charges). Both types of ion interactions (long-range van der Waals or short-range ionic hydration) strongly affect the magnitude of the double layer interaction, and can account for the specific ion effects observed experimentally. However, they do not affect qualitatively the traditional theory of the colloid stability, which predicts that the colloid is stable when there is a sufficiently large charge on the surface, and coagulates when the van der Waals interactions between two colloidal particles dominate. The only qualitative difference found when the ion-dispersion interactions were incorporated into the traditional double layer theory was the emergence of a 'double layer attraction' at very large separations, which, however, does not affect much the stability of colloids.
The technique of diffusive gradients in thin films (DGT) has been suggested to sample an available fraction of metals in soil. The objectives of this study were to compare DGT measurements with commonly measured fractions of Zn in soil, viz, the soil solution concentration and the total Zn concentration. The DGT technique was used to measure fluxes and interfacial concentrations of Zn in three series of field-contaminated soils collected in transects toward galvanized electricity pylons and in 15 soils amended with ZnCl2 at six rates. The ratio of DGT-measured concentration to pore water concentration of Zn, R, varied between 0.02 and 1.52 (mean 0.29). This ratio decreased with decreasing distribution coefficient, Kd, of Zn in the soil, which is in agreement with the predictions of the DGT-induced fluxes in soils (DIFS) model. The R values predicted with the DIFS model were generally larger than the observed values in the ZnCl2-amended soils at the higher Zn rates. A modification of the DIFS model indicated that saturation of the resin gel was approached in these soils, despite the short deployment times used (2 h). The saturation of the resin with Zn did not occur in the control soils (no Zn salt added) or the field-contaminated soils. Pore water concentration of Zn in these soils was predicted from the DGT-measured concentration and the total Zn content. Predicted values and observations were generally in good agreement. The pore water concentration was more than 5 times underpredicted for the most acid soil (pH = 3) and for six other soils, for which the underprediction was attributed to the presence of colloidal Zn in the soil solution.
It is well-established that sampling and sample processing can easily introduce contamination into dissolved trace element samples if precautions are not taken. However, work in remote locations sometimes precludes bringing bulky clean lab equipment into the field and likewise may make timely transport of samples to the lab for processing impossible. Straightforward syringe filtration methods are described here for collecting small quantities (15 mL) of 0.45- and 0.02-microm filtered river water in an uncontaminated manner. These filtration methods take advantage of recent advances in analytical capabilities that require only small amounts of waterfor analysis of a suite of dissolved trace elements. Filter clogging and solute rejection artifacts appear to be minimal, although some adsorption of metals and organics does affect the first approximately 10 mL of water passing through the filters. Overall the methods are clean, easy to use, and provide reproducible representations of the dissolved and colloidal fractions of trace elements in river waters. Furthermore, sample processing materials can be prepared well in advance in a clean lab and transported cleanly and compactly to the field. Application of these methods is illustrated with data from remote locations in the Rocky Mountains and along the Yukon River. Evidence from field flow fractionation suggests that the 0.02-microm filters may provide a practical cutoff to distinguish metals associated with small inorganic and organic complexes from those associated with silicate and oxide colloids.