Thesis (MScEng)--Stellenbosch University. / ENGLISH ABSTRACT: Carbon dioxide (CO2) is classified as the main greenhouse gas (GHG) contributing to global warming. Estimates by the Intergovernmental Panel on Climate Change (IPCC) suggest that CO2 emissions must be reduced by between 50 to 85% by 2050 to avoid irreversible impacts. Carbon capture and storage (CCS) strategies can be applied to de-carbonize the emissions from fossil-fueled power plants. Compared to other CCS techniques, post-combustion capture (PCC) is most likely to be implemented effectively as a retrofit option to existing power plants. At present however CCS is not yet commercially viable. The main challenge with CCS is to reduce the inherent energy penalty of the CO2 separation stage on the host plant. Seventy-five to eighty percent of the total cost of CCS is associated with the separation stage. There are several technologies available for separating CO2 from power plant flue gas streams. Reactive absorption with aqueous amine solutions has the ability to treat low concentration, low pressure and large flux flue gas streams in industrial-scale applications. It is most likely to be the first technology employed commercially in the implementation of CCS. The energy required for solvent regeneration however, is high for the standard solvent used in reactive absorption processes, i.e. MEA. This leads to a reduction in thermal efficiency of the host plant of up to 15%. Alternative solvent formulations are being evaluated in an attempt to reduce the energy intensity of the regeneration process. The main objective of this study was to establish a novel, simplified thermodynamic method for solvent screening. Partial solubility parameters (PSPs) were identified as the potential basis for such a method. The major limitation of this approach is that the model doesn’t account for effects from chemical reaction(s) between materials, e.g. CO2 reacting with aqueous alkanolamine solutions; considering only the effects from dissolution. The EquiSolv software system was developed based on PSP theory. The Hansen 3-set PSP approach was used to describe the equilibrium behaviour of CO2 absorbing in task specific solvents. The Hansen theory was expanded to a 4-set approach to account for contributions from electrostatic interactions between materials. The EquiSolv program was used successfully to screen large sets of solvent data (up to 400 million formulations) in the search for suitable alternative solvent formulations for CO2 absorption. The secondary objective of this study was to evaluate the ability of the proposed PSP model to accurately predict suitable alternative solvents for CO2 absorption through preliminary experimental work. A series of CO2 absorption experiments were conducted to evaluate the absorption performance of predicted alternative solvent formulations. The predicted alternative solvent formulations exhibited a significant improvement in absorption performance (up to a 97% increase in the measured absorption capacity) compared to conventional solvent formulations. Statistical analysis of the experimental results has shown that there is a statistically significant concordant relationship between the predicted and measured rankings for the absorption performance of the predicted solvent formulations. Based on this it was concluded that PSP theory can be used to accurately predict the equilibrium behaviour of CO2 absorbing in task specific solvents. Recently ionic liquids (ILs) have been identified as potential alternatives to alkanolamine solutions conventionally used for CO2 absorption. Absorption experiments were conducted as a preliminary assessment of the absorption performance of ILs. Results have shown ILs to have significantly improved performance compared to conventional alkanolamine solvents; up to a 96% increase in the measured absorption capacity compared to conventional solvents. Future work should focus on developing task specific ionic liquids (TSILs) in an attempt to reduce the energy intensity of solvent regeneration in CO2 absorption processes. / AFRIKAANSE OPSOMMING: Koolsuurgas (CO2) word geklassifiseer as die vernaamste kweekhuis gas (GHG) wat bydra to globale verwarming. Beramings deur die Interregeringspaneel oor Klimaatsverandering (IPKV) toon aan dat CO2 emissies teen 2050 verminder moet word met tussen 50 en 85% om onomkeerbare invloede te vermy. Verskeie koolstof opvangs en bergings (KOB) strategieë kan toegepas word ten einde die koolstof dioksied konsentrasie in die emissies van kragstasies wat fossielbrandstowwe gebruik, te verminder. Naverbranding opvangs (NVO) is die mees aangewese KOB tegniek wat effektief toegepas kan word op bestaande kragstasies. Tans is KOB egter nog nie kommersieël lewensvatbaarvatbaar nie. Die hoof uitdaging wat KOB in die gesig staar is om die energie boete inherent aan die CO2 skeidingstap te verminder. Tussen vyf-en-sewentig en tagtig persent van die totale koste van KOB is gekoppel aan die skeidingstap. Daar is verskeie metodes beskikbaar vir die skeiding van CO2 uit die uitlaatgasse van kragstasies. Reaktiewe absorpsie met waterige oplossings van amiene kan gebruik word om lae konsentrasie, lae druk en hoë vloei uitlaatgasstrome in industriële toepassings te behandel. Dit is hoogs waarskynlik die eerste tegnologie wat kommersieël aangewend sal word in die toepassing van KOB. Die oplosmiddel wat normalweg vir reaktiewe absorpsie gebruik word (d.w.s. MEA) benodig egter ‘n groot hoeveelheid energie vir regenerasie. Dit lei tot ‘n afname in die termiese doeltreffendheid van die voeder aanleg van tot 15%. Alternatiewe oplosmiddelstelsels word tans ondersoek in ‘n poging om the energie intensiteit van die regenerasieproses te verminder. Die hoof doelwit van hierdie studie was om ‘n nuwe, ongekompliseerde termodinamiese metode te vestig vir die keuring van alternatiewe oplosmiddels. Parsiële oplosbaarheidsparameters (POPs) is geïdentifiseer as ‘n moontlike grondslag vir so ‘n metode. Die model beskryf egter slegs die ontbindings gedrag van materiale. Die effekte van chemise reaksie(s) tussen materiale, bv. die tussen CO2 en waterige oplossings van alkanolamiene, word nie in ag geneem nie. Die POP teorie het gedien as grondslag vir die ontwerp van die EquiSolv sagteware stelsel. Die Hansen stel van drie POPs is gebruik om die ewewigsgedrag te beskryf van CO2 wat absorbeer in doelgerig-ontwerpte oplosmiddels. Die Hansen teorie is verder uitgebrei na ‘n stel van vier POPs om die bydrae van elektrostatiese wisselwerking tussen materiale in ag te neem. Die EquiSolv program is verskeie kere met groot sukses gebruik vir die sifting van groot stelle data (soveel as 400 miljoen formulasies) in die soektog na alternatiewe oplosmiddels vir CO2 absorpsie. Die sekondêre doelwit van die studie was om die vermoë van die voorgestelde POP model om geskikte alternatiewe oplosmiddels vir CO2 absorpsie akkuraat te voorspel, te ondersoek deur voorlopige eksperimentele werk. ‘n Reeks CO2 absorpsie eksperimente is gedoen ten einde die absorpsie werkverrigting van die voorspelde alternatiewe oplosmidels te ondersoek. ‘n Verbetering in absorpsie werkverrigting van tot 97% is gevind vir die voorspelde oplosmiddels vergeleke met die van oplosmiddels wat tipies in die industrie gebruik word. Statistiese ontleding van die eksperimentele resultate het getoon dat daar ‘n beduidende ooreenstemming tussen die voorspelde en gemete rangskikking van die voorspelde oplosmiddels se werkverrigting bestaan. Dus kan POP teorie gebruik word om die absorpsie van CO2 in doelgerig-ontwerpte oplosmiddels akkuraat te beskryf. Ioniese vloeistowwe (IVs) is onlangs geïdentifiseer as moontlike alternatiewe oplosmidels vir die alkanolamien oplossings wat normaalweg gebruik word vir CO2 absorpsie. Absorpsie eksperimente is gedoen ten einde ‘n voorlopige raming van die absorpsie werkverrigting van IVs te bekom. Daar is bevind dat IVs ‘n beduidende verbetering in werkverrigting toon in vergelyking met die alkanolamien oplosmiddels wat normaalweg gebruik word. ‘n Verbetering in absorpsie werkverrigting van tot 96% is gevind vir die voorspelde IV-bevattende oplosmiddels vergeleke met die van oplosmiddels wat tipies in die industrie gebruik word. Die fokus van toekomstige navorsing moet val op die ontwikkeling van doelgemaakte ioniese vloeistowwe (DGIVs) in ‘n poging om die energie intensiteit van oplosmiddel regenerasie in CO2 absorpsie prosesse te verminder.

This dissertation presents a fibre-optic sensing approach to provide continuous measurements of CO2 concentration at discrete points under typical conditions of geological CO2 storage. Carbon capture and storage is considered to have potential for a large-scale reduction in CO2 emissions in a relatively short period of time while other solutions to replace fossil fuels are being investigated. One significant drawback of carbon capture and storage is the possibility of long-term CO2 leakage. Therefore, the development of reliable technology for monitoring, verification, and accounting of geological CO2 storage is critical to fulfill safety regulations and achieve public acceptance. The major limitations of current technology include relatively low resolutions, high costs, and the lack of continuous monitoring for long periods of time. To address these limitations, two types of fibre-optic sensors are investigated, namely long period gratings and Mach-Zehnder interferometers. The sensing principle for CO2 detection is based on the sensitivity of these sensors to the refractive index of the medium that surrounds the fibre. Fibre-optic sensors are attractive for downhole applications due to the possibility of fabricating inexpensive high resolution devices that are able to operate in harsh environments over long periods of time. This dissertation focuses on increasing the refractive index sensitivity of long period gratings and Mach-Zehnder interferometers by applying coatings that have a high refractive index. The dip-coating method is used to coat long period gratings with polystyrene, and the sensitivity at low refractive indices is increased by tuning coating thickness. The results show that long period gratings coated with polystyrene are able to detect CO2 in gaseous and aqueous media. This work reports the first measurement of CO2 dissolution in water at high pressure with a fibre-optic sensor. Additionally, atomic layer deposition is investigated to coat long period gratings and Mach-Zehnder interferometers with hafnium oxide. The study of this coating technique aims to address the main limitation of the dip-coating method: the challenge to achieve precise control over coating thickness. The results show that atomic layer deposition is suitable to maximize the sensitivity of long period gratings and Mach-Zehnder interferometers at a target refractive index. / Graduate / 0548 / 0752 / 0799 / luismelo@uvic.ca

No description available.

Global warming along with the climate change derived from the World's demand for energy are among the greatest challenges to our society. To tackle climate change issue, research must focus on proposing practical approaches for carbon emissions reduction and environmental remediation. This thesis focuses on carbon dioxide separation mainly from flue gases (major sources of carbon dioxide emissions) using metal organic frameworks (MOFs) to reduce its impact on the global warming hence the climate change. MOFs are a class of crystalline porous adsorbents with structures that attract CO2 selectively and store it in their porous frameworks. Over the course of this PhD research, the fundamental aspects of these materials, as well as their practical applications, have been investigated. For example, the synthesis recipe of copper (II) benzene-1,3,5-tricarboxylate (CuBTC) MOF was improved to deliver a product of high yield ( > 89%) and free of by-product. Also, a mechanism study on the hydrothermal stability CuBTC MOF was carried out under simulated flue gas conditions and delivered the first experimental proof of the decomposition mechanism of CuBTC MOF caused by the water vapour. The fundamental understanding of the stability of materials then motivated the research into the development of a facile method of using an economic functional dopant (i.e. glycine) to strengthen the structure of CuBTC MOF (completely stable towards water vapour), as well as to improve the selectivity of resulting materials to CO2 (by 15% in comparison to the original CuBTC MOF). The suitability of the CuBTC MOF for fixed bed adsorption processes was also assessed using a combined experimental and process simulation method. In addition to the experimental approaches, molecular simulation based on grand canonical Monte Carlo method was also used to understand the effect of structural defects of MOFs on the CO2 adsorption isotherms.

The cryogenic carbon capture™ (CCC) process provides energy- and cost-efficient carbon capture and can be configured to provide an energy storage system using an open-loop natural gas (NG) refrigeration system, which is called energy storing cryogenic carbon capture (CCC-ES™). This investigation focuses on the transient operation and especially on the dynamic response of this energy storage system and explores its efficiency, effectiveness, design, and operation. This investigation included four tasks.The first task explores the steady-state design of four different natural gas liquefaction processes simulated by Aspen HYSYS. These processes differ from traditional LNG process in that the CCC process vaporizes the LNG and the cold vapors return through the LNG heat exchangers, exchanging sensible heat with the incoming flows. The comparisons include costs and energy performance with individually optimized processes, each operating at three operating conditions: energy storage, energy recovery, and balanced operation. The second task examines steady-state and transient models and optimization of natural gas liquefaction using Aspen HYSYS. Steady-state exergy and heat exchanger efficiency analyses characterize the performance of several potential systems. Transient analyses of the optimal steady-state model produced most of the results discussed here. The third task explores transient Aspen HYSYS modeling and optimization of two natural gas liquefaction processes and identifies the rate-limiting process components during load variations. Novel flowrate variations included in this investigation drive transient responses of all units, especially compressors and heat exchangers. Model-predictive controls (MPC) effectively manages such heat exchangers and compares favorably with results using traditional controls. The last task shows how an unprocessed natural gas (NG) pretreatment system can remove more than 90% of the CO2 from NG with CCC technology using Aspen Plus simulations and experimental data. This task shows how CCC-based technology can treat NG streams to prepare them for LNG use. Data from an experimental bench-scale apparatus verify simulation results. Simulated results on carbon (CO2) capture qualitatively and quantitatively agree with experimental results as a function of feedstock properties.

Green chemistry principles have been applied to the enhancement of two industrial chemistry problems. An industrially used reaction to form alcohols from aldehydes and ketones, the Meerwein-Ponndorf-Verley reduction, was improved by introducing a new catalyst Al(OtBu)₃. Due to the lower state of aggregation of this catalyst versus the conventional Al(OiPr)₃ catalyst, reduction rates were found to be faster in both pure iPrOH and mixed solvent systems for three model compounds: benzaldehyde, acetophenone, and a complex, chiral ketone, (S)-CMK. This allowed for the successful implementation of two important milestones; lowering the amount of catalyst needed necessary to complete the reactions (an economic benefit and lower waste) and the conversion from traditional batch reactions to continuous flow (a processing benefit) whereby reactions can be scaled-out rather than scaled-up. Another industrially important field of research that was focused on was CO₂ capture. High energy demands from current CO₂ capture methods such as aqueous amine solvents, specifically from coal-fired power plant flue gas, led to the development of non-aqueous reversible ionic liquids based on silylated amines. Structural modifications of the substitution around the silicon atom, the length of the alkyl chain bonding the silicon and amine, branching along the alkyl backbone, and investigating secondary and primary amines within this class of silylated amines were completed. These amines were reacted with CO₂ and the CO₂ capacity, the ionic liquid viscosity, reversal temperature and reaction enthalpy were all considered as a function of structure. In all cases the capacity was found to be not only greater than that of monethanolamine, an industrial standard, but higher than theoretical predictions through the formation of carbamic acid. Viscosity, reversal temperature, and reaction enthalpy were all found to be tunable through structure. These modifications gave significant insight into the necessary direction for optimization of these solvents as energy-efficient replacements of current CO₂ capture technology.

The Intergovernmental Panel on Climate Change (2001) reports that increased anthropogenic greenhouse gas (GHG) emissions, of which carbon dioxide (CO2) is the main component, have caused the Earths temperature to rise. Therefore, it is necessary to find ways to reduce GHG emissions and to deal with the emissions that continue to be produced. Carbon capture and storage (CCS) is one method that is being considered to deal with GHG emissions, specifically CO2 emissions. The basic idea behind CCS is that CO2 is captured from a point source, such as a power plant, and is then transported to a storage site (e.g., an oil or gas reservoir), where it is subsequently stored. The International Energy Agency Greenhouse Gas Programme (IEA GHG) began a CO2 geological sequestration pilot project in 2000 in Weyburn, Saskatchewan as part of an enhanced oil recovery project operatedby Cenovus (formerly EnCana) in the Weyburn Field (White et al. 2004). The research presented in this thesis evaluates the sealing potential of the Lea Park Formation in the Weyburn Field by determining its permeability and CO2 breakthrough pressure. In this context, breakthrough pressure describes the differential pressure between a wetting phase (e.g., formation brine) and a non-wetting phase (e.g., CO2) that is sufficient to enable the non-wetting phase to form a connected flow system across a given volume of porous medium (e.g., a rock sample). A new system for measuring the permeability and CO2 breakthrough pressure of shales was developed in this research. The development effort included extensive trouble-shooting and, ultimately, the development of sample preparation and testing procedures. The new system was used to conduct permeability and CO2 breakthrough pressure tests on shale samples from the Lea Park Formation (i.e., Lea Park shale) and the Colorado Group (i.e., Colorado shale). Permeability results for samples from the Lea Park shale ranged from 14 to 35 nd (1410-21 to 3510-21 m2), and between eight and 46 nd (810-21 to 4610-21 m2) for the Colorado shale. A CO2 breakthrough pressure for the Lea Park shale was determined to be 0.02 MPa, while values of 0.02 and 2.7 MPa were measured for the Colorado shale. The CO2 breakthrough pressure test results indicate that the Lea Park shale will not withstand large pressures before allowing CO2 to flow through it. However, the permeabilities are extremely low; hence the rate of flow would be low. In other words, the low permeability of the Lea Park shale will be the controlling factor in terms of the rate of potential CO2 leakage through it. Calculations based on the properties measured in this research suggest that the time required for CO2 to flow from the base to the top of the Lea Park Formation would be on the order of ten thousand years. Based on diffusion coefficients published for other shales, calculations suggest that CO2 leakage via chemical diffusion would be several times slower leakage via hydraulically-driven flow.

Optimal operation of plants is becoming more important due to increasing competition and small and changing profit margins for many products. One major reason has been the realization by industry that potentially large savings can be achieved by improving processes. Growth rates and profitability are much lower now, and international competition has increased greatly. The industry is faced with a need to manufacture quality products, while minimizing production costs and complying with a variety of safety and environmental regulations. As industry is confronted with the challenge of moving toward a clearer and more sustainable path of production, new technologies are needed to achieve industrial requirements. In this research, a new methodology is proposed to integrate so-called new technologies into existing processes. Research shows that the new technologies must be carefully selected and adopted to match the complex requirements of an existing process. The new proposed methodology is based on four major steps. If the improvement in the process is not sufficient to meet business needs, new technologies can be considered. Application of a new technology is always perceived as a potential threat; therefore, financial risk assessment and reliability risk analysis help alleviate risk of investment. An industrial case study from the literature was selected to implement and validate the new methodology. The case study is a planning problem to plan the layout or design of a fleet of generating stations owned and operated by the electric utility company, Ontario Power Generation (OPG). The impact of new technology integration on the performance of a power grid consisting of a variety of power generation plants was evaluated. The reduction in carbon emissions is projected to be accomplished through a combination of fuel switching, fuel balancing and switching to new technologies: carbon capture and sequestration. The fuel-balancing technique is used to decrease carbon emissions by adjusting the operation of the fleet of existing electricity-generating stations; the technique of fuel-switching involves switching from carbon-intensive fuels to less carbon-intensive fuels, for instance, switching from coal to natural gas; carbon capture and sequestration are applied to meet carbon emission reduction requirements. Existing power plants with existing technologies consist of fossil fuel stations, nuclear stations, hydroelectric stations, wind power stations, pulverized coal stations and a natural gas combined cycle, while hypothesized power plants with new technologies include solar stations, wind power stations, pulverized coal stations, a natural gas combined cycle and an integrated gasification combined cycle with and without capture and sequestration. The proposed methodology includes financial risk management in the framework of a two stage stochastic programme for energy planning under uncertainty: demands and fuel price. A deterministic mixed integer linear programming formulation is extended to a two-stage stochastic programming model in order to take into account random parameters, which have discrete and finite probabilistic distributions. Thus, the expected value of the total costs of power generation is minimized, while the objective of carbon emission reduction is achieved. Furthermore, conditional value at risk (CVaR), a most preferable risk measure in the financial risk management, is incorporated within the framework of two-stage mixed integer programming. The mathematical formulation, which is called mean-risk model, is applied for the purpose of minimizing expected value. The process is formulated as a mixed integer linear programming model, implemented in GAMS (General Algebraic Modeling System) and solved using the CPLEX algorithm, a commercial solver embedded in GAMS. The computational results demonstrate the effectiveness of the proposed new methodology. The optimization model is applied to an existing Ontario Power Generation (OPG) fleet. Four planning scenarios are considered: a base load demand, a 1.0% growth rate in demand, a 5.0% growth rate in demand, a 10% growth rate in demand and a 20% growth rate in demand. A sensitivity analysis study is accomplished in order to investigate the effect of parameter uncertainties, such as uncertain factors on coal price and natural gas price. The optimization results demonstrate how to achieve the carbon emission mitigation goal with and without new technologies, while minimizing costs affects the configuration of the OPG fleet in terms of generation mix, capacity mix and optimal configuration. The selected new technologies are assessed in order to determine the risks of investment. Electricity costs with new technologies are lower than with the existing technologies. 60% CO2 reduction can be achieved at 20% growth in base load demand with new technologies. The total cost of electricity increases as we increase CO2 reduction or increase electricity demand. However, there is no significant change in CO2 reduction cost when CO2 reduction increases with new technologies. Total cost of electricity increases when fuel price increases. The total cost of electricity increases with financial risk management in order to lower the risk. Therefore, more electricity is produced for the industry to be on the safe side.

Optimal operation of plants is becoming more important due to increasing competition and small and changing profit margins for many products. One major reason has been the realization by industry that potentially large savings can be achieved by improving processes. Growth rates and profitability are much lower now, and international competition has increased greatly. The industry is faced with a need to manufacture quality products, while minimizing production costs and complying with a variety of safety and environmental regulations. As industry is confronted with the challenge of moving toward a clearer and more sustainable path of production, new technologies are needed to achieve industrial requirements. In this research, a new methodology is proposed to integrate so-called new technologies into existing processes. Research shows that the new technologies must be carefully selected and adopted to match the complex requirements of an existing process. The new proposed methodology is based on four major steps. If the improvement in the process is not sufficient to meet business needs, new technologies can be considered. Application of a new technology is always perceived as a potential threat; therefore, financial risk assessment and reliability risk analysis help alleviate risk of investment. An industrial case study from the literature was selected to implement and validate the new methodology. The case study is a planning problem to plan the layout or design of a fleet of generating stations owned and operated by the electric utility company, Ontario Power Generation (OPG). The impact of new technology integration on the performance of a power grid consisting of a variety of power generation plants was evaluated. The reduction in carbon emissions is projected to be accomplished through a combination of fuel switching, fuel balancing and switching to new technologies: carbon capture and sequestration. The fuel-balancing technique is used to decrease carbon emissions by adjusting the operation of the fleet of existing electricity-generating stations; the technique of fuel-switching involves switching from carbon-intensive fuels to less carbon-intensive fuels, for instance, switching from coal to natural gas; carbon capture and sequestration are applied to meet carbon emission reduction requirements. Existing power plants with existing technologies consist of fossil fuel stations, nuclear stations, hydroelectric stations, wind power stations, pulverized coal stations and a natural gas combined cycle, while hypothesized power plants with new technologies include solar stations, wind power stations, pulverized coal stations, a natural gas combined cycle and an integrated gasification combined cycle with and without capture and sequestration. The proposed methodology includes financial risk management in the framework of a two stage stochastic programme for energy planning under uncertainty: demands and fuel price. A deterministic mixed integer linear programming formulation is extended to a two-stage stochastic programming model in order to take into account random parameters, which have discrete and finite probabilistic distributions. Thus, the expected value of the total costs of power generation is minimized, while the objective of carbon emission reduction is achieved. Furthermore, conditional value at risk (CVaR), a most preferable risk measure in the financial risk management, is incorporated within the framework of two-stage mixed integer programming. The mathematical formulation, which is called mean-risk model, is applied for the purpose of minimizing expected value. The process is formulated as a mixed integer linear programming model, implemented in GAMS (General Algebraic Modeling System) and solved using the CPLEX algorithm, a commercial solver embedded in GAMS. The computational results demonstrate the effectiveness of the proposed new methodology. The optimization model is applied to an existing Ontario Power Generation (OPG) fleet. Four planning scenarios are considered: a base load demand, a 1.0% growth rate in demand, a 5.0% growth rate in demand, a 10% growth rate in demand and a 20% growth rate in demand. A sensitivity analysis study is accomplished in order to investigate the effect of parameter uncertainties, such as uncertain factors on coal price and natural gas price. The optimization results demonstrate how to achieve the carbon emission mitigation goal with and without new technologies, while minimizing costs affects the configuration of the OPG fleet in terms of generation mix, capacity mix and optimal configuration. The selected new technologies are assessed in order to determine the risks of investment. Electricity costs with new technologies are lower than with the existing technologies. 60% CO2 reduction can be achieved at 20% growth in base load demand with new technologies. The total cost of electricity increases as we increase CO2 reduction or increase electricity demand. However, there is no significant change in CO2 reduction cost when CO2 reduction increases with new technologies. Total cost of electricity increases when fuel price increases. The total cost of electricity increases with financial risk management in order to lower the risk. Therefore, more electricity is produced for the industry to be on the safe side.

The Intergovernmental Panel on Climate Change (2001) reports that increased anthropogenic greenhouse gas (GHG) emissions, of which carbon dioxide (CO2) is the main component, have caused the Earths temperature to rise. Therefore, it is necessary to find ways to reduce GHG emissions and to deal with the emissions that continue to be produced. Carbon capture and storage (CCS) is one method that is being considered to deal with GHG emissions, specifically CO2 emissions. The basic idea behind CCS is that CO2 is captured from a point source, such as a power plant, and is then transported to a storage site (e.g., an oil or gas reservoir), where it is subsequently stored. The International Energy Agency Greenhouse Gas Programme (IEA GHG) began a CO2 geological sequestration pilot project in 2000 in Weyburn, Saskatchewan as part of an enhanced oil recovery project operatedby Cenovus (formerly EnCana) in the Weyburn Field (White et al. 2004). The research presented in this thesis evaluates the sealing potential of the Lea Park Formation in the Weyburn Field by determining its permeability and CO2 breakthrough pressure. In this context, breakthrough pressure describes the differential pressure between a wetting phase (e.g., formation brine) and a non-wetting phase (e.g., CO2) that is sufficient to enable the non-wetting phase to form a connected flow system across a given volume of porous medium (e.g., a rock sample). A new system for measuring the permeability and CO2 breakthrough pressure of shales was developed in this research. The development effort included extensive trouble-shooting and, ultimately, the development of sample preparation and testing procedures. The new system was used to conduct permeability and CO2 breakthrough pressure tests on shale samples from the Lea Park Formation (i.e., Lea Park shale) and the Colorado Group (i.e., Colorado shale). Permeability results for samples from the Lea Park shale ranged from 14 to 35 nd (1410-21 to 3510-21 m2), and between eight and 46 nd (810-21 to 4610-21 m2) for the Colorado shale. A CO2 breakthrough pressure for the Lea Park shale was determined to be 0.02 MPa, while values of 0.02 and 2.7 MPa were measured for the Colorado shale. The CO2 breakthrough pressure test results indicate that the Lea Park shale will not withstand large pressures before allowing CO2 to flow through it. However, the permeabilities are extremely low; hence the rate of flow would be low. In other words, the low permeability of the Lea Park shale will be the controlling factor in terms of the rate of potential CO2 leakage through it. Calculations based on the properties measured in this research suggest that the time required for CO2 to flow from the base to the top of the Lea Park Formation would be on the order of ten thousand years. Based on diffusion coefficients published for other shales, calculations suggest that CO2 leakage via chemical diffusion would be several times slower leakage via hydraulically-driven flow.