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Geochemical Reactions in Unsaturated Mine WastesJerz, Jeanette K. 26 April 2002 (has links)
Although mining is essential to life in our modern society, it generates huge amounts of waste that can lead to acid mine drainage (AMD). Most of these mine wastes occur as large piles that are open to the atmosphere so that air and water vapor can circulate through them. This study addresses the reactions and transformations of the minerals that occur in humid air in the pore spaces in the waste piles.
The rate of pyrite oxidation in moist air was determined by measuring over time the change in pressure between a sealed chamber containing pyrite plus oxygen and a control. The experiments carried out at 25?C, 96.8% fixed relative humidity, and oxygen partial pressures of 0.21, 0.61, and 1.00 showed that the rate of oxygen consumption is a function of oxygen partial pressure and time. The rates of oxygen consumption fit the expression (dn/dt=(3.31x10^-7)(P^0.5)(t^-0.5)
It appears that the rate slows with time because a thin layer of ferrous sulfate + sulfuric acid solution grows on pyrite and retards oxygen transport to the pyrite surface.
The transformation of efflorescent sulfate minerals (the reaction products of iron sulfide oxidation) from a pyrrhotite-rich massive sulfide is explained using a systematic analysis of their stoichiometry and thermodynamics. Their stabilities are controlled by oxygen partial pressure, relative humidity, and activity of sulfuric acid and can be visualized using log activity of oxygen-log activity of water and log acitvity of sulfuric acid-log activity of water diagrams developed during this study.
Samples from the field site were analyzed in the laboratory to determine mineralogy, equilibrium relative humidity, chemical composition, and acid generation potential. Dissolution experiments showed that fibroferrite-rich samples had the highest acid producing potential, followed by copiapite-rich samples and then halotrichite-rich samples. The most abundant metals in solutions produced by dissolving the salts were magnesium, aluminum, zinc, copper, calcium, and lead. The molar concentrations of the metals varied with mineralogy. However, all of these minerals release metals and acid when they dissolve and therefore represent a significant environmental threat. / Ph. D.
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Effects of Exercise Training on Fat Oxidation in Untrained Overweight and Obese FemalesManning, Kelly 11 August 2011 (has links)
This study examined whether a high-intensity interval (IT) or a continuous steady-state (CT) exercise training program had the greatest effect on fat oxidation rates and fat mass loss in a population of untrained overweight and obese females. Thirteen female subjects (VO2peak 30.6 ± 1.29 ml.kg.min-1, BMI 29 ± 0.79, fat mass [FM] 33.3 ± 2.09 kg) were randomly assigned to either a CT (exercise at the relative intensity that elicits the maximal fat oxidation rate [FATmax] ) or an IT (intervals alternating 5 minutes at 40% and 85% VO2peak) training group that exercised approximately 1 hour, 3 days.week-1 for 10 weeks. Body composition assessments, peak oxygen uptake (VO2peak), FATmax and plasma free fatty acid (FFA) concentrations were examined pre- and post-training using dual-energy X-ray absorptiometry (DEXA), ParvoMedics gas analysis system and FFA half micro tests (Roche Diagnostics). No significant differences were found post-training in body weight (kg), body fat (%), fat-free mass, or fat mass (P>0.05). The relative exercise intensity that elicited FATmax was significantly increased from 35.3 ± 2.55% to 44.7 ± 3.56% in the IT group post-training (P <0.05). The maximal fat oxidation rate was determined at a higher relative exercise intensity after 10 weeks of a IT program compared with a CT program, which resulted in longer durations of fat oxidation during submaximal exercise bouts. These data suggest that an IT program induces a greater increase in the relative exercise intensity that elicits maximal fat oxidation after 10 weeks of training compared to a CT program in this population. Although body composition and FATmax were not altered, it is possible that through training induced metabolic adaptations from the IT program, intramuscular triacylglyceride (IMTG) contributions to fat oxidation at a given steady-state work rate could be increased post-training.
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Modeling the Effect of Thermal Oxidation on the Pore Structure of Artificial GraphitePaul, Ryan Michael 08 September 2011 (has links)
No description available.
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Oxidation of Graphite and Metallurgical Coke : A Numerical Study with an Experimental ApproachAhmad, Yousef January 2016 (has links)
At the royal institute of technology (KTH) in the department of applied process metallurgy, a novel modelling approach has been developed which allows a dynamic coupling between the commercial thermodynamic software Thermo-Calc and the commercial computational fluid dynamic (CFD) software Ansys Fluent, only referred to as Fluent in the study. The dynamic coupling approach is used to provide numerical CFD-models with thermodynamic data for the thermo-physical properties and for the fluid-fluid chemical reactions occurring in metallurgical processes. The main assumption forthe dynamic coupling approach is the existence of local equilibrium in each computational cell. By assuming local equilibrium in each computational cell it is possible to use thermodynamic data from thermodynamic databases instead of kinetic data to numerically simulate chemical reactions. The dynamic coupling approach has been used by previous studies to numerically simulate chemical reactions in metallurgical processes with good results. In order to validate the dynamic coupling approach further, experimental data is required regarding surface reactions. In this study, a graphiteand metallurgical coke oxidation experimental setup was suggested in order to provide the needed experimental data. With the experimental data, the ability of the dynamic couplings approach to numerically predict the outcome of surface reactions can be tested.By reviewing the literature, the main experimental apparatus suggested for the oxidationexperiments was a thermo-gravimetric analyzer (TGA). The TGA can provide experimental data regarding the reaction rate, kinetic parameters and mass loss as a function of both temperature and time. An experimental setup and procedure were also suggested.In order to test the ability of Fluent to numerically predict the outcome of surface reactions, without any implementation of thermodynamic data from Thermo-Calc, a benchmarking has been conducted. Fluent is benchmarked against graphite oxidation experiments conducted by Kim and No from the Korean advanced institute of science and technology (KAIST). The experimental graphite oxidation rates were compared with the numerically calculated graphite oxidation rates obtained from Fluent. A good match between the experimental graphite oxidation rates and the numerically calculated graphite oxidation rates were obtained. A parameter study was also conducted in order to study the effect of mass diffusion, gas flow rate and the kinetic parameters on the numerically calculated graphite oxidation rate. The results of the parameter study were partially supported by previous graphite oxidation studies. Thus, Fluent proved to be a sufficient numerical tool for numerically predicting the outcome of surface reactions regarding graphite oxidation at zero burn-off degree.
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Oxidation and Textural Characteristics of Butter and Ice Cream with Modified Fatty Acid ProfilesGonzalez, Sonia 16 August 2001 (has links)
Milk fat composition determines specific rheological, sensory and physicochemical properties of dairy products such as texture, melting point, flavor, color, oxidation rates, and viscosity. Previous studies have shown that milkfats containing higher levels of long chain polyunsaturated fatty acids have lower melting points and decreased solid fat contents which leads to softer-textured products. An increased risk of higher oxidation rates can be a disadvantage of high levels of polyunsaturated fatty acids.
Three different milkfat compositions were obtained through dietary manipulation of cows: high oleic content, high linoleic content and control milkfat. Ice cream and butter were processed from the treated and control milks. Butter and ice cream samples then were analyzed to measure differences in fatty acid profiles and firmness. High-oleic and high-linoleic milkfat had lower concentrations of saturated fatty acids, such as C 16:0. Conjugated linoleic acid content was increased in the high-linoleic milkfat. High-oleic milkfat resulted in a softer butter. Ice cream samples were analyzed to measure differences in viscosity, melting point, oxidation rate and sensory perception. Significant differences (P<0.05) were found in the fatty acid profiles of milkfat, ice cream mix viscosity, peroxide values of ice cream after 3 to 5 months of storage, butter color, and butter firmness. Sensory analyses included a scooping test at -18°C to detect differences in texture. A difference test was conducted to determine oxidation flavor differences between the three ice cream treatments at extended storage times. No significant differences were found in the scooping test or the oxidation flavor difference.
Manipulation of the cow's diet increased the total amount of unsaturated fatty acids. It also influenced firmness of butter and behavior of peroxide values during extended storage of high-linoleic ice cream. / Master of Science
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Resolving the atmospheric sulphur budget over the Elandsfontein area of the Mpumalanga HighveldIgbafe, Anselm Iuebego 02 September 2008 (has links)
A novel study on the investigation of three very common atmospheric sulphur species
relevant to the Mpumalanga Highveld subregion was conducted. Long-term in situ
measurements were applied in the diurnal and seasonal evaluation of the observed sulphur
species. Ambient pollutant concentrations and surface meteorological data were collected
at an air quality monitoring station at Elandsfontein. Elandsfontein air quality monitoring
station was ideal for the observations due to its high elevation within the Mpumalanga
Province surrounded by few rolling hills and negligible windbreaks which easily allows for
extensive plume-contact with the surface during convective daytime mixing. The temporal
characteristics of the sulphur species have been assessed relative to one another with
varying meteorological conditions. The diurnal and seasonal concentration variations were
used to describe the physical characteristics exhibited by the compounds over
Elandsfontein. Pollution roses were used to target the source of the major release points
and areas of these sulphur species relative to the Elandsfontein monitoring station. Gas and
particle concentrations were analysed in relation to varying meteorological parameters with
a view to ascertaining the sulphur transformation and concentration distribution in the
planetary boundary layer. Particulate sulphate distribution has been modelled through
multivariate regression analyses in relation to three meteorological parameters, namely,
wind speed, relative humidity and ambient temperature for the various seasons observed
over southern Africa.
This study has shown that hydrogen sulphide, sulphur dioxide and sulphate species are
present throughout the year in the Mpumalanga Highveld at notably significant levels. The
presence of ambient particulate sulphate has been shown to result from the combination of
chemical interactions during long-range aerosol transport; atmospheric recirculation
processes shown from back trajectories over the southern Africa sub-region, as well as the
variation in the removal mechanisms and rates for the different seasons throughout the
year. These transport and removal processes all contribute to the overall sulphur mass
balance in the planetary boundary layer. Dosage of the three sulphur species was evaluated
to provide data for sulphur pollution loading that could form a basis for health and
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environmental impact assessments over the area. In view of the characteristic patterns
displayed by particulate sulphate, multivariate mathematical models have been developed
on a seasonal basis with variations in meteorological parameters. This was seen to predict
an accuracy of up to 70 % of the particulate sulphate loading for different seasons over the
South African Highveld.
In order to understand the chemical interactions of atmospheric sulphur species, it is
important to be able to predict the route taken and expected products of transformation on
any given condition. Theoretical analyses of the chemical thermodynamic properties of the
known reacting species and a well-established approach were used in predicting reaction
paths and establishing the possible and feasible products of chemical transformation in
relation to the ambient temperature. The determination of reaction paths and possible
products of chemical transformation provides a measure of the relative importance of the
reacting species and the mechanism of reaction. Gas-, aqueous-phase and radical reactions
involving sulphur (IV) were investigated with a view to establishing their relative
importances. Thermochemical properties of several sulphur-containing compounds not
available in the literature have been generated for evaluation of Gibbs free energy (ΔG)
and enthalpy (ΔH). An electronic energy structural approach has been applied to model for
ΔG and ΔH of 88 sulphur species in 90 chemical reactions comprising gas-phase, aqueousphase
and radical reactions. Modelling was evaluated for their relative importances over a
temperature range of –100 °C to +100 °C. The temperature range is well above the known
tropospheric temperature range to account for variations in the atmospheric environment.
To further comprehend the chemistry of sulphur with regards to distribution of the species
in the atmosphere, a kinetic model is developed and incorporated into a dispersion model.
The kinetic evaluation of the oxidation rate of SO2 to sulphate has been determined with
advection and dispersion over the Elandsfontein area. Gas-phase transformation with
advection and dispersion has been used to evaluate the extent of the distribution of SO2
relative to the major contributing sources. The dry deposition was considered to be the
dominant removal mechanism. It was assumed that the reaction rate was second order in
concentration and that the rate of deposition was first order. The oxidation rates obtained
for the seasons were 10.9 % h-1 for summer; 8.83 % h-1 for autumn; 6.56 % h-1 for winter;
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10.8 % h-1 for spring, while an overall rate of 9.6 % h-1 was obtained for the one year study
period. The transformation rate model produced a reaction constant and an activation
energy of 4.92 x 10-6 μg m-3 s-1 and 36.54 kJ kg-1 for summer; 3.939 x 10-6 μg m-3 s-1
and 43.89 kJ kg-1 for autumn; 2.90 x 10-6 μg m-3 s-1 and 115.69 kJ kg-1 for winter;
4.82 x 10-6 μg m-3 s-1 and 43.29 kJ kg-1 for spring, while for the year
4.29 x 10-6 μg m-3 s-1 and 34.31 kJ kg-1. A Gaussian puff unsteady state Lagrangian
dispersion model with reflection at the surface and inversion layer was applied for
concentration diffusion. The Lagrangian dispersion model with dry deposition was a better
prediction of the observed data than the models from previous studies using a first order
rate constant with or without deposition rate.
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Stress corrosion cracking and internal oxidation of alloy 600 in high temperature hydrogenated steam and waterLindsay, John Christopher January 2015 (has links)
In this study, the possibility of using low pressure hydrogenated steam to simulate primary water reactor conditions is examined. The oxides formed on Alloy 600 (WF675) between 350 Celsius and 500 Celsius in low pressure hydrogenated steam (with a ratio of oxygen at the Ni/NiO to oxygen in the system of 20) have been characterised using analytical electron microscopy (AEM) and compared to oxide that formed in a high pressure water in a autoclave at 350 Celsius with 30 cc/kg of hydrogen. Preferential oxidation of grain boundaries and bulk internal oxidation were observed on samples prepared by oxide polishing suspension (OPS). Conversely, samples mechanically ground to 600 grit produced a continuous, protective oxide film which suppressed the preferential and internal oxidation. The surface preparation changed the form of the oxides in both steam and autoclave tests. The preferential oxidation rate has been determined to be K_{oxide} = Aexp{-Q/RT}with A = 2.27×10^(−3) m^(2)s^(−1) and Q = 221 kJ.mol^(−1) (activation energy) for WF675 and A = 5.04 × 10^(−7) m^(2)s^(−1) and Q = 171 kJ.mol^(−1) for 15% cold worked WF675. These values are consistent with the activation energy of primary water stress corrosion cracking (PWSCC) initiation. Bulk oxygen diffusivities were calculated from the internal oxidation after 500 h exposures. At 500 Celsius the oxygen diffusivity was determined to be 1.79×10^(−20) m^(2)s^(−1) for WF675 and 1.21×10^(−20) m^(2)s^(−1) for 15% cold worked WF675, the oxygen diffusivity at 400 Celsius in 15% cold worked WF675 was calculated to be 1.49×10^(−22) m^(2)s^(−1).The Cr-depletion associated with preferential oxidation has been assessed by AEM. The Cr-depletion was asymmetric and it could not be accounted for by local variations in the diffusion rate. Chemically induced grain boundary migration is suggested as a possible explanation. Constant load SCC tests conducted in hydrogenated steam at 400 Celsius have shown a similar trend to the classical dependency of PWSCC as a function of potential. The SCC samples were also prepared with two surface finishes, OPS and 600 grit. In all SCC tests, significantly more cracking was observed on the OPS surface and all failures initiated from this surface.
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