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<p> In this study the experiments were designed to measure the geochemical and surface charge (zeta potential) changes with time for two crushed samples of feldspar (Na-fs and K-fs) over the pH range of most natural waters (5 to 9). These experiments show: </p> <p> (a) the importance of adsorption/desorption phenomena in both short-term and long-term feldspar dissolution, and probably for chemical weathering in general; </p> <p> (b) that the generalized curve which characterizes the geochemical data (an initial rapid rise to a peak followed by a decrease to a lower, either constant or later increasing value) is consistent with a consideration of the adsorption/desorption process (i.e., the formation of the double layer) taking place at the feldspar surface and with the simple dissolution of the mineral; </p> <p> (c) that the cation-silica ratios (Na₂O/SiO₂, K₂O/SiO₂, CaO/SiO₂) of the solution compared to those in the original feldspar indicate an initially incongruent dissolution which tends towards congruency during the latter part of the experiments. </p> <p> From information in the Iiterature and the results of these experiments. it may be concluded that: </p> <p> (a) the most important or master variables in chemical weathering are abrasion, minerologic or crystallographic factors such as twinning, exsolution regions, impurities, fractures and grain size, and solution composition and concentration. pH does not appear to be a master variable in most natural waters, especially for long-term weathering, and the chemical composition of the mineral phase is also not a good criterion for predicting weathering behaviour; and </p> <p> (b) the most extreme chemical weathering should occur in a high energy environment, either for physical reasons (i.e., high abrasion due to extreme relief) or for chemical reasons (i.e., high rainfall). </p> / Thesis / Master of Science (MSc)

京都大学 / 新制・課程博士 / 博士(農学) / 甲第25320号 / 農博第2586号 / 京都大学大学院農学研究科森林科学専攻 / (主査)教授 髙野 俊幸, 教授 上髙原 浩, 教授 和田 昌久 / 学位規則第4条第1項該当 / Doctor of Philosophy (Engineering) / Kyoto University / DGAM

La thèse traite du transport de particules colloïdales en milieu poreux. L'influence des propriétés physico-chimiques et hydrodynamiques sur le dépôt et détachement de particules de latex a été étudiée en réalisant des expériences durant lesquelles des grandeurs macroscopiques (concentration dans les effluents, réduction de perméabilité) et microscopiques (variation de porosité par atténuation gamma) ont été mesurées. / This thesis deals with colloidal particle transport in porous media. The influence of physicochemical and hydrodynamic conditions on the deposition and detachment of latex particles was studied by performing a series of experiments during which macroscopic (effluent concentration, permeability reduction) and microscopic (porosity variation) properties were measured.

Adsorption/desorption behaviors of three volatile organic compounds (VOCs) emitted from the optoelectronics industry by Y-type and ZSM-5 zeolites were studied in this work. Target VOCs include acetone, isopropyl alcohol (IPA), and propylene glycol monomethyl ether acetate (PGMEA). Adsorption/desorption experiments were conducted in a fixed-bed column using various operating conditions to mimic the commercial ones. Also studied include the adsorption kinetics for single-component, two-component, and three-component cases. Experimental results of the single-adsorbate case by both model zeolites have shown that the amount of VOC adsorbed follows the order of PGMEA > IPA > Acetone. This is ascribed to the greatest molecular weight of PGMEA among three VOCs tested. The adsorption capacity of each zeolite for each target VOC was found to increase with its increasing initial concentration. Freundlich isotherm and Langmuir isotherm were found to be suitable for describing the adsorption behaviors for the single-adsorbate case. Results of the desorption experiments also showed that most of the target VOCs could be desorbed at 180¢J in 100 minutes. The adsorption capacities of the regenerated model zeolites were found to be decreasing as the regeneration times increased. As compared with the fresh ones, the regenerated zeolites had reduced specific surface areas, but increased pore sizes. In addition, the Yoon and Nelson equation was employed to study the kinetic behaviors of adsorbing the target VOCs by the model zeolites. A good agreement of the experimental results and predictions by the Yoon & Nelson model was obtained for the single-adsorbate case. However, the Yoon and Nelson model was found to be incompetent to simulate and predict all the multi-adsorbate cases including two-component adsorption and three-component adsorption in this work. Again, it is speculated that the displacement of lower-molecular-weight adsorbates (i.e., acetone and IPA) by PGMEA (an adsorbate of a much greater molecular weight) would be responsible for this finding. For the two-adsorbate case, nevertheless, the Yoon and Nelson equation was found to be capable of describing the adsorption behavior under the circumstance of C/C0 < 1.

Trends show that the fraction of the world's population with electronic devices using modern integrated circuits is increasing at a rapid rate. To meet consumer demands: less expensive, faster, and smaller electronics; while still making a profit, manufacturers must shrink transistor dimensions while increasing the number of transistors per integrated circuit; a trend predicted by Gorden E. Moore more than 44 years prior. As CMOS transistors scale down in size, new techniques such as atomic-layer deposition (ALD) are used to grow features one atomic layer at a time. ALD and other manufacturing processes are requiring increasingly stringent purities of process gases and liquids in order to minimize circuit killing defects which reduces yield and drives up manufacturing cost. Circuit killing defects caused by impurity incursions into UHP gas distribution system can come from a variety of sources and one of the impurity transport mechanisms investigated was back diffusion; the transport of impurities against convective flow. Once impurity incursions transpire, entire production lines are shut down and purging with UHP gas is initiated; a process that can take months thus resulting in tens of millions of dollars in lost revenue and substantial environment, safety, and health (ESH) impacts associated with high purge gas consumption. A combination of experimental investigation and process simulation was used to analyze the effect of various operational parameters on impurity back diffusion into UHP gas distribution systems. Advanced and highly sensitive analytical equipment, such as the Tiger Optics MTO 1000 H2O cavity ring-down spectrometer (CRDS), was used in experiments to measure real time back diffusing moisture concentrations exiting an electro-polished stainless-steel (EPSS) UHP distribution pipe. Design and operating parameters; main and lateral flow rates, system pressure, restrictive flow orifice (RFO) aperture size, and lateral length were changed to impact the extent of back diffusing impurities from a venting lateral. The process model developed in this work was validated by comparing its predictions with data from the experiment test bed. The process model includes convection, molecular diffusion in the bulk, surface diffusion, boundary layer transport, and all modes of dispersion; applicable in both laminar and turbulent flow regimes. Fluid dynamic properties were directly measured or were obtained by solving Navier-Stokes and continuity equations. Surface diffusion as well as convection and dispersion in the bulk fluid played a strong role in the transport of moisture from vents and lateral branches into the main line. In this analysis, a dimensionless number (Peclet Number) was derived and applied as the key indicator of the relative significance of various transport mechanisms in moisture back-diffusion. Guidelines and critical values of Peclet number were identified for assuring the operating conditions meet the purity requirements at the point of use while minimizing UHP gas usage. These guidelines allowed the determination of lateral lengths, lateral diameters, flow rates, and restrictive flow device configurations to minimize contamination and UHP gas consumption. Once a distribution system is contaminated, a significant amount of purge time is required to recover the system background due to the strong interactions between moisture molecules and the inner surfaces of the components in a gas distribution system. Because of the very high cost of UHP gases and factory downtime, it is critical for high-volume semiconductor manufacturers to reduce purge gas usage as well as purge time during the dry-down process. The removal of moisture contamination in UHP gas distribution systems was approached by using a novel technique dubbed pressure cyclic purge (PCP). EPSS piping was contaminated with moisture, from a controlled source, and then purged using a conventional purge technique or a PCP technique. Moisture removal rates and overall moisture removal was determined by measuring gas phase moisture concentration in real time via a CRDS moisture analyzer. When compared to conventional purge, PCP reduced the time required and purge gas needed to clean the UHP gas distribution systems. However, results indicate that indiscriminately initiating PCP can have less than ideal or even detrimental results. An investigation of purge techniques on the removal of gas phase, chemisorbed, and physisorbed moisture, coupled with the model predictions, led to the testing of hybrid PCP. The hybrid PCP approach proved to be the most adaptable purge technique and was used in next phase of testing and modeling. Experiments and modeling progressed to include testing the effectiveness of hybrid PCP in systems with laterals; more specifically, laterals that are "dead volumes" and results show that hybrid PCP becomes more purge time and purge gas efficient in systems with increasing number and size of dead volumes. The process model was used as a dry-down optimization tool requiring inputs of; geometry and size, temperature, starting contamination level, pressure swing limits of inline equipment, target cleanliness, and optimization goals; such as, minimizing pure time, minimizing purge gas usage, or minimizing total dry-down cost.

Techn. Universiẗat, Diss., 2002--Darmstadt.

For this dissertation I studied phosphorus (P) sorption dynamics in the shallow groundwater of the southern Everglades. In particular, I examined how the ambient water type governs soluble reactive P (SRP) availability through adsorption/desorption reactions with the aquifer matrix. Chapter 2 investigated how P sorption dynamics of the mangrove root zone sediment are affected by high bicarbonate brackish groundwater compared to both fresh groundwater and saltwater. The results from chapter 2 show that the sediment exhibited exceptionally low sorption efficiency in the high bicarbonate brackish water, which would allow ambient water SRP concentration to be maintained at a higher level. Chapter 3 is a detailed analysis of how P sorption dynamics in two bedrock samples are affected by incremental increases in saltwater content in a freshwater-saltwater transition zone. The results of chapter 3 indicate that a sorption edge occurs at 3 mM Cl- concentration. In water exceeding this Cl- concentration, SRP would be expected to desorb from the bedrock due to a sharp decrease in sorption efficiency between the freshwater saltwater. These results suggest that SRP is active in the ion exchange front of saltwater intrusion, with a rapid increase in SRP availability expected at the leading edge of saltwater intrusion. A landward incursion of 3 mM Cl- concentration water would be expected to raise ambient SRP concentration along the affected aquifer zone, in turn increasing SRP availability in the ecosystem where the transitional waters discharge to the surface. Chapter 4 investigates the kinetics SRP release accompanying saltwater intrusion using a column of carbonate aquifer solids and alternating inflow between fresh groundwater and saltwater. The results show an immediate and high magnitude increase in SRP concentration when saltwater flows into the column. The combined results of this dissertation show that, in the southern Everglades and possibly other carbonate coastlines as well, water type strongly controls P sorption behavior of the sediment and bedrock, and may have a direct influence on the local ecology through increased P availability. A fundamental understanding of the abiotic exchange mechanisms between SRP and the aquifer solids can aid in the successful management and protection of this unique and important ecosystem.

M. Tech (Department of Chemistry, Faculty of Applied and Computer Sciences) Vaal University of Technology. / Persisting challenges associated with remediation of heavy metals from aqueous media have stirred the need for enhancement of current technologies. Cellulosic agro waste materials (AWM) as well as ion-imprinted polymers (IIP) have received ardent attention from researchers. These materials are often employed in the following industries: water and wastewater treatment, medical, pharmaceutical and packaging. Applications in water and wastewater treatment have gained significant interest due to desirable features they possess. In the case of AWM, these features include a tuneable surface area and poor porosity, basic surface functional groups and chemical stability. Some desired features in IIP include adsorption sites compatible for the ion imprint obtained after leaching with suitable reagents, rigidity and reusability. The efficacy of employing AWM and IIP for the remediation of toxic chromium from aqueous solution was explored. The current study is made up of part A and B. In part A, Macadamia nutshell powder was treated using HNO3, NaOH, as well as Fenton’s reagent. The three materials underwent a new modification which involved reacting treated adsorbents with cetyltrimethylammonium chloride (CTAC), followed by immobilization of 1,5' diphenylcarbazide (DPC) ligand. The adsorbents were ultimately washed, dried and stored for Cr(VI) batch adsorption experiments. Part B involved a synthesis of IIP and their non-imprinted polymer counterpart (NIP) for Cr(VI) sequestration in aqueous solution. This was done by precipitation polymerization of functional monomers, crosslinker and DPC-Cr(VI) complex as a template. Non-imprinted polymers were fashioned in a manner like that of IIP but with the exclusion of Cr(VI) ion template. Characterizations of the adsorbents were done using Fourier transform infrared spectroscopy (FTIR), thermogravimetric analysis (TGA), scanning electron microscopy (SEM), X-ray fluorescence (XRF), and carbon, hydrogen, nitrogen and sulphur (CHNS) analyzer. Batch adsorption experiments were done and parameters such as solution pH, adsorbent dosage, initial Cr(VI) concentration and contact time were optimized. Working solutions were analyzed using ultraviolet-visible (UV-Vis) and atomic absorption (AA) spectroscopy. Adsorption parameters found to be optimum for DPC immobilized cellulosic adsorbents were pH 1.4, adsorbent mass of 0.1 g, 100 mg/L initial concentration and 125 minutes of contact time. The adsorption parameters determined to be optimum for IIP and NIP were pH 2.6, 0.2 g adsorbent mass, 80 mg/L initial concentration and 240 minutes of contact time. Reusability studies demonstrated the potential of adsorbents to remove Cr(VI) ions from aqueous media after successive adsorption-desorption cycles. Selectivity studies indicated that DPC immobilized adsorbents as well as IIP were able to selectively adsorb Cr(VI) ions from aqueous media in the presence of Zn(II), Cu(II), Co(II) and NI(II) ions. Kinetic models revealed that DPC immobilized cellulosic adsorbents and synthetic IIP were most fitting for pseudo-second order and pseudo first order, respectively. On the other hand, adsorption isotherm studies demonstrated that DPC immobilized cellulosic adsorbents and synthetic polymers were best fit for Freundlich and Langmuir adsorption isotherm, respectively.

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