Hydrogen is known as a clean energy carrier which has the potential to play a major role in addressing the climate change and global warming, and thermochemical water splitting via the copper-chlorine cycle is a promising method of hydrogen production. In this research, thermal management of the copper-chlorine cycle for hydrogen production is investigated by performing analytical and experimental analyses of selected heat recovery options. First, the heat requirement of the copper-chlorine cycle is estimated. The pinch analysis is used to determine the maximum recoverable heat within the cycle, and where in the cycle the recovered heat can be used efficiently. It is shown that a major part of the potential heat recovery can be achieved by cooling and solidifying molten copper(I) chloride exiting one step in the cycle: the oxygen reactor. Heat transfer from molten CuCl can be carried out through direct contact or indirect contact methods. Predictive analytical models are developed to analyze a direct contact heat recovery process (i.e. a spray column) and an indirect contact heat recovery process (i.e. a double-pipe heat exchanger). Characteristics of a spray column, in which recovered heat from molten CuCl is used to produce superheated steam, are presented. Decreasing the droplet size may increase the heat transfer rate from the droplet, and hence decreases the required height of the heat exchanger. For a droplet of 1 mm, the height of the heat exchanger is predicted to be about 7 m. The effect of hydrogen production on the heat exchanger diameter was also shown. For a hydrogen production rate of 1000 kg/day, the diameter of the heat exchanger is about 3 m for a droplet size of 1 mm and 2.2 m for a droplet size of 2 mm. The results for axial growth of the solid layer and variations of the coolant temperature and wall temperature of a double-pipe heat exchanger are also presented. It is shown that reducing the inner tube diameter will increase the heat exchanger length and increase the outlet temperature of air significantly. It is shown that the air temperature increases to 190oC in a heat exchanger with a length of 15 cm and inner tube radius of 10 cm. The length of a heat exchanger with the inner tube radius of 12 cm is predicted to be about 53 cm. The outlet temperature of air is about 380oC in this case. The length of a heat exchanger with an inner tube diameter of 24 cm is predicted to be about 53 cm and 91 cm for coolant flow rates of 3 g/s and 4 g/s, respectively. Increasing the mass flow rate of air will increase the total heat flux from the molten salt by increasing the length of the heat exchanger. Experimental studies are performed to validate the proposed methods and to further investigate their feasibility. The hazards involving copper(I) chloride are also investigated, as well as corresponding hazard reduction options. Using the reactant Cu2OCl2 in the oxygen production step to absorb CuCl vapor is the most preferable option compared to the alternatives, which include absorbing CuCl vapor with water or CuCl2 and building additional structures inside the oxygen production reactor. / UOIT

Clearwells are large water reservoirs often used at the end of the water treatment process as chlorine contact chambers. Contact time required for microbe destruction is provided by residence time within the clearwell. The residence time distribution can be determined from tracer tests and is the one of the key factors in assessing the hydraulic behaviour and efficiency of these reservoirs. This work provides an evaluation of whether the two-dimensional, depth-averaged, finite element model, River2DMix can adequately simulate the flow pattern and residence time distribution in clearwells. One question in carrying out this modelling is whether or not the structural columns in the reservoir need to be included, as inclusion of the columns increases the computational effort required.<p> In this project, the residence time distribution predicted by River2DMix was compared to results of tracer tests in a scale model of the Calgary Glenmore water treatment plant northeast clearwell. Results from tracer tests in this clearwell were available. The clearwell has a serpentine baffle system and 122 square structural columns distributed throughout the flow. A comparison of the flow patterns in the hydraulic and computational models was also made. The hydraulic model tests were carried out with and without columns in the clearwell.<p> The 1:19 scale hydraulic model was developed on the basis of Froude number similarity and the maintenance of minimum Reynolds numbers in the flow through the serpentine system and the baffle wall at the entrance to the clearwell. Fluorescent tracer slug injection tests were used to measure the residence time distribution in the clearwell. Measurements of tracer concentration were taken at the clearwell outlet using a continuous flow-through fluorometer system. Flow visualization was also carried out using dye to identify and assess the dead zones in the flow. It was found that it was necessary to ensure the flow in the scale model was fully developed before starting the tracer tests, and determining the required flow development time to ensure steady state results from the tracer tests became an additional objective of the work. Tests were carried out at scale model flows of 0.85, 2.06, and 2.87 L/s to reproduce the 115, 280, and 390 ML/day flows seen in the prototype tracer tests.<p> Scale model results of the residence time distribution matched the prototype tracer test data well. However, approximately 10.5 hours was required for flow development at the lowest flow rate tested (0.85 L/s) before steady state conditions were reached and baffle factor results matched prototype values. At the intermediate flow, baffle factor results between the scale model and prototype matched well after only 1 h of flow development time, with improvements only in the Morril dispersion index towards prototype values with increased flow development time (at 5 h). Similar results were seen at the highest flow tested. For fully developed flow, there was little change in the baffle factor and dispersion index results in the scale model with varied flow rate.<p> With the addition of columns to the scale model, there was no significant change in the baffle factor compared to the case compared to without the columns, but up to a 13.9 % increase in dispersion index as compared to the tests in the scale model without columns for fully developed flow. Further, the residence time distribution results from the scale model tests without columns matched the entire residence time distribution found in the prototype tests. However, for the model with columns, the residence time distribution matched the prototype curve well at early times, but departed significantly from it at times later in the tests. It appears the major effect of the addition of columns within a model clearwell is to increase the dispersion index and increase the proportion of the clearwell which operates as a mixed reactor.<p> The results also showed there was good agreement between the physical model tests and River2DMix simulations of the scale model tests for both the flow pattern and residence time distributions. This indicates that a two-dimensional depth-averaged computer model such as River2DMix can provide representative simulation results in the case where the inlet flow is expected to be quickly mixed throughout the depth of flow in the clearwell.

Chlorine is an essential building block in the environment and can be found in most places. Chlorine participates in a complex biogeochemical cycle and has been discussed for many years and it is well documented that natural chlorination of organic compound takes place in many parts of the ecosystem. Chlorine can be inorganic (Clin) and organically bound (Clorg). Previous studies have shown that the transformation of Clin to Clorg is connected with the amount of organic matter and the microbial activity in the soil. So far, studies have been focused on forest soil and there is a need for analysing the natural chlorination in other soil types. The aim of this study was to provide chlorination rates in agricultural soil which does not weem to have been done previously. Three common agricultural soils experiencing different agricultural practice and different cropping systems were incubated with Na36Cl at 20o C in a 56 days radiotracer experiment. The results show that a chlorination of 36Clin to 36Clorg in agricultural soil occurred and the Clorg levels increased over time. The chlorination rates ranged from 0,040 to 0,063 μg Cl g dry weight soil-1 d1. This was 10-fold lower than rates previously measured in coniferous forest soil. However, when expressed as μg Cl g dry weight organic carbon-1 d-1, rates in the agricultural soil was only slightly (at the most 2-fold) lower than in coniferous forest. This study contributes with new knowledge of natural chlorination rates in agricultural soil and gives further evidence that the natural chlorination can be connected to the amount of organic matter in the soil.

The Atmospheric Chemistry Experiment (ACE) is a satellite mission for remote sensing of the Earth's atmosphere using the solar occultation technique. The primary instrument on this satellite is the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS). ACE-FTS retrievals are described with a focus on the creation of <em>a priori</em> temperature and pressure profiles. ACE-FTS measurements are then used to investigate the chemistry, transport and trends of chlorine, fluorine and water in the stratosphere, leading to an improved understanding of processes affecting both stratospheric ozone depletion and global climate change. <br /><br /> Total chlorine (Cl_TOT) in the stratosphere is determined using ACE-FTS measurements of eleven chlorine-containing species, supplemented by both other measurements and models, to determine Cl_TOT as a function of altitude in five latitude zones. All resulting Cl_TOT profiles are nearly linear, with a slight slope. Mean Cl_TOT for 2004 is determined to be 3. 65 ppbv for both the northern and southern midlatitudes (with a precision and estimated accuracy of ±0. 09 and ±0. 13 ppbv, respectively). A slightly lower value of mean Cl_TOT is determined for the tropics and slightly higher values at high latitudes. Total fluorine (F_TOT) in the stratosphere is also determined primarily from ACE-FTS measurements using a similar approach, resulting in stratospheric F_TOT profiles which are nearly linear with mean values ranging from 2. 50 to 2. 59 ppbv for each latitude zone (with a precision of 0. 04-0. 07 ppbv and an estimated accuracy of 0. 15 ppbv). The observed slopes and pattern of latitudinal variation are evidence of the beginning of a decline in global stratospheric chlorine and of the continuing increase in global stratospheric fluorine levels. <br /><br /> The abundance of water in the stratosphere is investigated for the northern hemisphere midlatitudes in 2004 using ACE-FTS measurements. Potential water is determined as [H₂O]+2[CH₄] and from [H₂O] versus [CH₄] correlations, resulting in a value of 7. 14±0. 05 ppmv, which is used to determine a value of 3. 65±0. 15 ppmv for the mean abundance of water entering the stratosphere. Both values are compared directly with historical data from the Atmospheric Trace Molecule Spectroscopy (ATMOS) instrument (1985-1994) and show a negligible change, implying that the increases observed by ATMOS and other long-term measurements from that time period have not continued. <br /><br /> The removal of stratospheric water in the Arctic vortex is investigated using ACE-FTS measurements. Using derived quantities from a meteorological data assimilation, northern hemisphere occultations from early 2004 are classified as vortex, vortex edge or extravortex. [CH₄] versus [N₂O] correlations are used to further classify the extravortex occultations as tropical, subtropical or midlatitude. Comparisons between profiles of [N₂O], [CH₄] and [H₂O] inside and outside the Arctic vortex, give estimates of upper stratospheric and lower mesospheric descent rates, indicating that descent in the winter 2004 Arctic vortex was rapid, with evidence of descent at higher altitudes than in past years. <br /><br /> The dehydration of air in the tropical tropopause layer and mechanisms for the entry of water vapor into the stratosphere are investigated by an analysis of ACE-FTS profiles of temperature, water vapor and [HDO]/[H₂O]. Month-to-month comparisons for 2004 and 2005 reveal a clear pattern of seasonal variation and a correlation between minimum temperature and maximum HDO depletion. Further interpretation indicates that the gradual dehydration mechanism accompanied by lofting of ice particles in the tropical troposphere is the most likely explanation for the observed seasonal variation and the shape of the [HDO]/[H₂O] profiles.

Clearwells are large water reservoirs often used at the end of the water treatment process as chlorine contact chambers. Contact time required for microbe destruction is provided by residence time within the clearwell. The residence time distribution can be determined from tracer tests and is the one of the key factors in assessing the hydraulic behaviour and efficiency of these reservoirs. This work provides an evaluation of whether the two-dimensional, depth-averaged, finite element model, River2DMix can adequately simulate the flow pattern and residence time distribution in clearwells. One question in carrying out this modelling is whether or not the structural columns in the reservoir need to be included, as inclusion of the columns increases the computational effort required.<p> In this project, the residence time distribution predicted by River2DMix was compared to results of tracer tests in a scale model of the Calgary Glenmore water treatment plant northeast clearwell. Results from tracer tests in this clearwell were available. The clearwell has a serpentine baffle system and 122 square structural columns distributed throughout the flow. A comparison of the flow patterns in the hydraulic and computational models was also made. The hydraulic model tests were carried out with and without columns in the clearwell.<p> The 1:19 scale hydraulic model was developed on the basis of Froude number similarity and the maintenance of minimum Reynolds numbers in the flow through the serpentine system and the baffle wall at the entrance to the clearwell. Fluorescent tracer slug injection tests were used to measure the residence time distribution in the clearwell. Measurements of tracer concentration were taken at the clearwell outlet using a continuous flow-through fluorometer system. Flow visualization was also carried out using dye to identify and assess the dead zones in the flow. It was found that it was necessary to ensure the flow in the scale model was fully developed before starting the tracer tests, and determining the required flow development time to ensure steady state results from the tracer tests became an additional objective of the work. Tests were carried out at scale model flows of 0.85, 2.06, and 2.87 L/s to reproduce the 115, 280, and 390 ML/day flows seen in the prototype tracer tests.<p> Scale model results of the residence time distribution matched the prototype tracer test data well. However, approximately 10.5 hours was required for flow development at the lowest flow rate tested (0.85 L/s) before steady state conditions were reached and baffle factor results matched prototype values. At the intermediate flow, baffle factor results between the scale model and prototype matched well after only 1 h of flow development time, with improvements only in the Morril dispersion index towards prototype values with increased flow development time (at 5 h). Similar results were seen at the highest flow tested. For fully developed flow, there was little change in the baffle factor and dispersion index results in the scale model with varied flow rate.<p> With the addition of columns to the scale model, there was no significant change in the baffle factor compared to the case compared to without the columns, but up to a 13.9 % increase in dispersion index as compared to the tests in the scale model without columns for fully developed flow. Further, the residence time distribution results from the scale model tests without columns matched the entire residence time distribution found in the prototype tests. However, for the model with columns, the residence time distribution matched the prototype curve well at early times, but departed significantly from it at times later in the tests. It appears the major effect of the addition of columns within a model clearwell is to increase the dispersion index and increase the proportion of the clearwell which operates as a mixed reactor.<p> The results also showed there was good agreement between the physical model tests and River2DMix simulations of the scale model tests for both the flow pattern and residence time distributions. This indicates that a two-dimensional depth-averaged computer model such as River2DMix can provide representative simulation results in the case where the inlet flow is expected to be quickly mixed throughout the depth of flow in the clearwell.

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