Perovskita de LaFeO3 sintetizadas pelo método de Pechini foram avaliadas como catalisadores para a reação de oxidação parcial do metano. Foi impregnado níquel por via úmida como fase ativa em concentrações de 15 e 30 %, sobre as perovskitas, 15NLF e 30NLF, respectivamente, e o seu efeito foi avaliado para a mesma reação. Foi realizado análises termogravimétricas (TGA/DTGA) nos precursores da perovskitas, constatando a sua formação a 650 °C. A análise de microscopia de varredura (MEV) foi realizada nas amostras da perovskita pura, sendo que em uma delas foi realizada um banho de ultrassom para diminuir o tamanho de suas partículas e avaliar este efeito na reação de POM. Análises de difração de raio X (DRX) mostraram que todas as amostras apresentam as mesmas propriedades cristalográficas, sendo que, nas amostras contendo níquel, o metal apresentou-se na forma de NiO. O tamanho dos cristais, cálculado através da equação de Scherer, foi na ordem de 20 nm. Este resultado apontou que o níquel impregnado não participa da estrutura perovskita, mas sim está sobreposto a esta. Através da microscopia eletrônica de transmissão (TEM) foi possível visualizar a dispersão da fase ativa na superfície óxida e tamanhos de partículas na ordem de 20 nm. A redução a temperatura programada (TPR) apresentou as temperaturas de redução de espécies níquel e de ferro, presente na perovskita, e permitiu compreender a atuação das espécies Ni+2 e Fe0 na formação de H2 e CO. Os testes catalíticos foram realizados a 700ºC e 750°C, a pressão atmosférica, para uma vazão de alimentação de 200 cm3.min-1. Os testes cataliticos mostraram que a conversão de H2 dobrou para perovskita Ni/LaFeO3 em relação a LaFeO3. O catalisador 15NLF apresentou melhor estabilidade que o catalisador 30NLF para a reação. / LaFeO3 perovskite synthesized by the Pechini method were evaluated for the partial oxidation reaction of methane. Nickel was impregnated as the active phase in concentrations of 15 and 30%, on perovskites, 15NLF and 30NLF, respectively, and its effect was evaluated for the same reaction. Thermogravimetric analyzes (TGA / DTGA) were carried out on the perovskite precursors, confirming their formation at 650 °C. Scanning microscopy (SEM) was performed on pure perovskite samples, in one of them an ultrasonic bath was performed to reduce the size of its particles and to evaluate this effect in the POM reaction. X-ray diffraction (XRD) analyzes showed that all samples had the same crystallographic properties, and in the samples containing nickel, the metal was present as NiO. The size of the crystals, calculated through the Scherer equation, was in the order of 20 nm. This result pointed out that the impregnated nickel does not participate in the perovskite structure. Through transmission electron microscopy (TEM) it was possible to visualize the dispersion of the active phase on the oxide surface and particle sizes in the order of 20 nm. The programmed temperature reduction (TPR) showed the iron and nickel species reduction temperatures present in the perovskite, and allowed to understand the Ni+ 2 and Fe0 species in the H2 and CO formation. The catalytic tests were performed at 700 °C and 750 °C at atmospheric pressure for a flow rate of 200 cm3.min-1. The catalytic tests showed that the conversion of H2 doubled to perovskite Ni/LaFeO3 in relation to LaFeO3. 15NLF catalyst presented better stability than the 30NLF catalyst for the reaction.

The search for environmentally benign energy sources is becoming increasingly urgent. One such technology is fuel cells, e.g., the polymer electrolyte membrane (PEM) fuel cell which uses hydrogen as a fuel and emits only H2O. However, reforming hydrocarbon fuels to produce the needed hydrogen yields reformate streams containing CO2 as well as CO, which is toxic to the PEM fuel cell at concentrations above 100ppm. As the amount of CO permitted to reach the fuel cell increases, the performance of the PEM fuel cell decreases until it ultimately stops functioning. The water-gas-shift (WGS) reaction, CO + H2O <-> H2 + CO2, provides a method for extracting the energy from the toxic CO by converting it into usable H2 along with CO2 which can be tolerated by the fuel cell. Although a well established industrial process, alternate catalysts are sought for fuel cell application. Catalyst selection for the WGS reaction has, until recently, been based on trial-and-error screening of potential catalysts due to a lack of fundamental understanding of the catalyst's functioning. For this reason, we embarked on a deeper understanding of the molecular events involved in the WGS reaction such that a more systematic and theory-guided approach may be used to design and select catalysts more efficiently, i.e., rational catalyst design. The goal of this research was to develop a comprehensive predictive microkinetic model for the WGS reaction which is based solely on a detailed mechanism as well as theories of surface-molecule interactions (i.e., the transition-state theory) with energetic parameters determined a priori. This was followed by a comparison of the experimental results of sample catalysts to validate the model for various metal-based catalysts of interest including Cu, Fe, Ni, Pd, Pt, Rh, and Ru. A comprehensive mechanism of the plausible elementary reaction steps was compiled from existing mechanisms in the literature. These were supplemented with other likely candidates which are derivatives of those identified in the literature. Using established theories, we predicted the kinetics of each of the elementary reaction steps on metal catalysts of interest. The Unity Bond Index-Quadratic Exponential Potential Method (UBI-QEP) was used to predict the activation energies in both the forward and reverse direction of each step based solely on heats of chemisorption and bond dissociation energies of the species involved. The Transition State Theory (TST) was used to predict the pre-exponential factors for each step assuming an immobile transition state; however, the pre-exponential factors were adjusted slightly to ensure thermodynamic consistency with the overall WGS reaction. In addition, we have developed a new and powerful theoretical tool to gain further insight into the dominant pathways on a catalytic surface as reactants become products. Reaction Route (RR) Graph Theory incorporates fundamental elements of graph theory and electrical network theory to graphically depict and analyze reaction mechanisms. The stoichiometry of a mechanism determines the connectivity of the elementary reaction steps. Each elementary reaction step is viewed as a single branch with an assumed direction corresponding to the assumed forward direction of the elementary reaction step. The steps become interconnected via nodes which reflect the quasi-steady state conditions of the species represented by the node. A complete RR graph intertwines a series of routes by which the reactants may be converted to products. Once constructed, the RR graph may be converted into an electrical network by replacing, in the steady-state case, each elementary reaction step branch with a resistor and including the overall reaction as a power source where rate and affinity correspond to current and voltage, respectively. A simplification and reduction of the mechanism may be performed based on results from a rigorous De Donder affinity analysis as it correlates to Kirchhoff's Voltage Law (KVL), akin to thermodynamic consistency, coupled with quasi-steady state conditions, i.e., conservation of mass, analyzed using Kirchhoff's Current Law (KCL). Hence, given the elementary reaction step resistances, in conjunction with Kirchhoff's Laws, a systematic reduction of the network identifies the dominant routes, e.g., the routes with the lowest resistance, along with slow and quasi-equilibrium elementary reaction steps, yielding a simplified mechanism from which a predictive rate expression may possibly be derived. Here, we have applied RR Graph Theory to the WGS reaction. An 18-step mechanism was employed to understand and predict the kinetics of the WGS reaction. From the stoichiometric matrix for this mechanism, the topological features necessary to assemble the RR graph, namely the intermediate nodes, terminal nodes, empty reaction routes and full reaction routes, were enumerated and the graph constructed. The assembly of the RR graph provides a comprehensive overview of the mechanism. After reduction of the network, the simplified mechanism, comprising the dominant pathways, identified the quasi-equilibrium and rate-determining steps, which were used to determine the simplified rate expression which predicts the rate of the complete mechanism for different catalysts. Experimental investigations were conducted on the catalysts of interest to validate the microkinetic model derived. Comparison of the experimental results from the industrially employed catalysts (e.g., Cu, Ni, Fe, etc.) shows that the simplified microkinetic model sufficiently predicts the behavior of the WGS reaction for this series of catalysts with very good agreement. Other catalysis tested (Pt, Pd, Rh and Ru), however, had sufficient methanation activity that a direct comparison with WGS kinetics could not be made. In summary, we have developed a comprehensive approach to unravel the mechanism and kinetics of a catalytic reaction. The methodology described provides a more fundamental depiction of events on the surface of a catalyst paving the way for rational analysis and catalyst design. Illustrated here with the WGS reaction as an example, we show that the dominant RRs may be systematically determined through the application of rigorous fundamental constraints (e.g. thermodynamic consistency and mass conservation) yielding a corresponding explicit a priori rate expression which illustrates very good agreement not only with the complete microkinetic mechanism, but also the experimental data. Overall, RR graph theory is a powerful new tool that may become invaluable for unraveling the mechanism and kinetics of complex catalytic reactions via a common-sense approach based on fundamentals.

Perovskita de LaFeO3 sintetizadas pelo método de Pechini foram avaliadas como catalisadores para a reação de oxidação parcial do metano. Foi impregnado níquel por via úmida como fase ativa em concentrações de 15 e 30 %, sobre as perovskitas, 15NLF e 30NLF, respectivamente, e o seu efeito foi avaliado para a mesma reação. Foi realizado análises termogravimétricas (TGA/DTGA) nos precursores da perovskitas, constatando a sua formação a 650 °C. A análise de microscopia de varredura (MEV) foi realizada nas amostras da perovskita pura, sendo que em uma delas foi realizada um banho de ultrassom para diminuir o tamanho de suas partículas e avaliar este efeito na reação de POM. Análises de difração de raio X (DRX) mostraram que todas as amostras apresentam as mesmas propriedades cristalográficas, sendo que, nas amostras contendo níquel, o metal apresentou-se na forma de NiO. O tamanho dos cristais, cálculado através da equação de Scherer, foi na ordem de 20 nm. Este resultado apontou que o níquel impregnado não participa da estrutura perovskita, mas sim está sobreposto a esta. Através da microscopia eletrônica de transmissão (TEM) foi possível visualizar a dispersão da fase ativa na superfície óxida e tamanhos de partículas na ordem de 20 nm. A redução a temperatura programada (TPR) apresentou as temperaturas de redução de espécies níquel e de ferro, presente na perovskita, e permitiu compreender a atuação das espécies Ni+2 e Fe0 na formação de H2 e CO. Os testes catalíticos foram realizados a 700ºC e 750°C, a pressão atmosférica, para uma vazão de alimentação de 200 cm3.min-1. Os testes cataliticos mostraram que a conversão de H2 dobrou para perovskita Ni/LaFeO3 em relação a LaFeO3. O catalisador 15NLF apresentou melhor estabilidade que o catalisador 30NLF para a reação. / LaFeO3 perovskite synthesized by the Pechini method were evaluated for the partial oxidation reaction of methane. Nickel was impregnated as the active phase in concentrations of 15 and 30%, on perovskites, 15NLF and 30NLF, respectively, and its effect was evaluated for the same reaction. Thermogravimetric analyzes (TGA / DTGA) were carried out on the perovskite precursors, confirming their formation at 650 °C. Scanning microscopy (SEM) was performed on pure perovskite samples, in one of them an ultrasonic bath was performed to reduce the size of its particles and to evaluate this effect in the POM reaction. X-ray diffraction (XRD) analyzes showed that all samples had the same crystallographic properties, and in the samples containing nickel, the metal was present as NiO. The size of the crystals, calculated through the Scherer equation, was in the order of 20 nm. This result pointed out that the impregnated nickel does not participate in the perovskite structure. Through transmission electron microscopy (TEM) it was possible to visualize the dispersion of the active phase on the oxide surface and particle sizes in the order of 20 nm. The programmed temperature reduction (TPR) showed the iron and nickel species reduction temperatures present in the perovskite, and allowed to understand the Ni+ 2 and Fe0 species in the H2 and CO formation. The catalytic tests were performed at 700 °C and 750 °C at atmospheric pressure for a flow rate of 200 cm3.min-1. The catalytic tests showed that the conversion of H2 doubled to perovskite Ni/LaFeO3 in relation to LaFeO3. 15NLF catalyst presented better stability than the 30NLF catalyst for the reaction.

Made available in DSpace on 2017-07-10T15:14:47Z (GMT). No. of bitstreams: 1 Luiz Inacio Chaves.pdf: 1830089 bytes, checksum: 5146991baf6ffcd2929ea26b316d8b8d (MD5) Previous issue date: 2012-09-17 / The use of biomass as energy source is one of the most promising, because it contributes to reduce emissions of carbon dioxide in the atmosphere and allow the decentralized energy generation. Gasification is a technology of processing biomass energy into a gaseous biofuel of low calorific value. The gas can be used in Otto cycle engine for power generation in isolated communities. This study evaluated the capacity of the gasification gas in a fixed bed gasifier downtraft of two stages, the wood consumption, the efficiency of the gasifier and the gas consumption and efficiency in apower-generator Otto cycle. The gasifier use was a TERMOQUIP brand, model CD 40. The evaluated power-generator was a BRANCO brand, direct injection and power of 13 cv coupled to an electric generator of 5.5 cv. The gasification gas was injected into the engine mixed with the intake air. The generator was subjected to loads ranging from 0.5 kW to 2.5 kW, with the aid of a bank of electrical resistances. The production of gas from the gasifier and gas consumption by the motor were measured by means of a gasometer. The average gas production resulting from the gasification of wood presented during testing was 14.28 m³ h&#713; ¹. Wood consumption averaged 5.61 kg h&#713; ¹. The average yield of gas per unit weight was approximately 2.55 m3kg&#713; ¹. The gasification efficiency averaged 57.2%. When fed with synthesis gas, the output voltage of the generator was kept within the standards established by Companhia Paranaense de Energia (Copel, 2008), varying only between 221 and 223 V. For tests with the power-generator the best condition occurred for the highest load, 2.5 kW, where the gas consumption was about 10.6 m³ h&#713; ¹ and specific fuel consumption of 4.8 m³ kWh&#713;¹. For this condition, the average specific fuel consumption of equivalent wood was 1.9 kg kWh &#713; ¹ and the overall efficiency of power-generator was about 16.6%. / O uso da biomassa como fonte de energia é uma das formas mais promissoras, pois contribui para a redução das emissões de dióxido de carbono na atmosfera e possibilita a geração descentralizada de energia. A gaseificação é uma tecnologia de transformação energética da biomassa num biocombustível gasoso de baixo poder calorífico. O gás pode ser utilizado em motor ciclo Otto para geração de energia elétrica em comunidades isoladas. Este trabalho avaliou a capacidade de produção de gás de gaseificação em um gaseificador concorrente de leito fixo de dois estágios, o consumo de madeira, a eficiência do gaseificador, a eficiência e o consumo de gás num motor-gerador ciclo Otto. O gaseificador utilizado foi da marca TERMOQUIP, modelo CD 40. O motor-gerador avaliado foi da marca BRANCO, com injeção direta e potência de 13 cv acoplado a um gerador elétrico de 5,5 cv. O gás de gaseificação foi injetado no motor misturado com o ar de admissão. O gerador foi submetido a cargas que variaram entre 0,5 kW e 2,5 kW, com o auxílio de um banco de resistências elétricas. A produção de gás do gaseificador e o consumo de gás pelo motor foram medidos por meio de um gasômetro. A produção de gás média resultante da gaseificação de madeira apresentada durante os testes foi de 14,28 m³ h&#713;¹. O consumo de madeira apresentou uma média de 5,61 kg h&#713;¹. A média de rendimento de gás por unidade de massa foi de aproximadamente 2,55 m3 kg&#713;¹. A eficiência de gaseificação média foi de 57,2 %.Quando alimentado com gás de síntese, a tensão de saída do gerador se manteve dentro dos padrões estabelecidos pela Companhia Paranaense de Energia (COPEL, 2008), variando somente entre 221 e 223 V. Em relação aos testes com o motor-gerador, a melhor condição ocorreu para a maior carga, 2,5 kW, onde o consumo de gás foi cerca de 10,6 m³ h&#713;¹ e o consumo específico de combustível de 4,8 m³ kWh&#713;¹. Para essa condição, a média de consumo específico equivalente de madeira foi de 1,9 kg kWh&#713;¹e a eficiência global do motor-gerador foi de 16,6 %.

Mitigation of climate change and energy security are major driving forces for increased biomass utilization. The pulp and paper industry consumes a large proportion of the biomass worldwide including bark, wood residues, and black liquor. Due to the fact that modern mills have established infrastructure for handling and processing biomass, it is possible to lay foundation for future gasification based bio-refineries to poly-produce electricity, chemicals or bio-fuels together with pulp and paper products. There is a potential to export electricity or bio-fuels by improving energy systems of existing chemical pulp mills by integrating gasification technology. The present study investigates bio-fuel alternatives from the dry black liquor gasification (BLG) system with direct causticization and direct methane production from the catalytic hydrothermal gasification (CHG) system. The studied systems are compared with bio-fuel alternatives from the Chemrec BLG system and the improvements in the energy systems of the pulp mill are analyzed. The results are used to identify the efficient route based on system performance indicators e.g. material and energy balances to compare BLG systems and the conventional recovery boiler system, potential biofuel production together with biomass to biofuel conversion efficiency, energy ratios, potential CO2 mitigation combining on-site CO2 reduction using CO2 capture and potential CO2 offsets from biofuel use, and potential motor fuel replacement. The results showed that the dry BLG system for synthetic natural gas (SNG) production offers better integration opportunities with the chemical pulp mill in terms of overall material and energy balances. The biofuel production and conversion efficiency are higher in the CHG system than other studied configurations but at a cost of larger biomass import. The dry BLG system for SNG production achieved high biomass to biofuel efficiency and considerable biofuel production. The energy ratio is significant in the dry BLG (SNG) system with less biomass demand and considerable net steam production in the BLG island. The elimination of the lime kiln in the dry BLG systems resulted in reduced consequences of incremental biomass import and associated CO2 emissions. Hydrogen production in the dry BLG system showed the highest combined CO2 mitigation potential i.e. on-site CO2 capture potential and CO2 offset from biofuel replacing fossil fuel. The results also showed that the motor fuel replacement potential with SNG as compressed natural gas (CNG) replacing gasoline in the transport sector is significantly high in countries with large pulp industry. / QC 20120528

The research institute ETC in Piteå is working with energy technical research and development. Today, much work revolves around research about renewable sources for fuel. In one project, biomass such as wood pellet is heated up while producing synthesis gas. The synthesis gas is then analyzed using three different GC techniques. ETC wanted to be able to make all their analysis on one instrument and with a faster speed. They contacted the company Rowaco in Linköping for help with developing a method on FTIR for analysis of the synthesis gas and that has been the aim for this thesis. A method has been developed for analysis of water, carbon monoxide, carbon dioxide and methane. The results from this thesis show that the concentrations of the molecules in the synthesis gas are outside the calibration curved that has been made and that the high concentrations give much interference to other molecules. The thesis also shows that many areas in the spectrum from the process are roof absorbers and there is also a contamination of water and carbon dioxide in the system. Suggested improvements are to find the source for the contamination, to develop calibration points with higher concentrations, to reduce the length of the gas cell and to dilute the gas before entering the FTIR.

Increasing prices of crude oil derived transportation fuels ascended the researches on seeking alternative fuels, in last decades. Moreover, the increasing rate of global warming, because of high greenhouse gas emissions initiated new research for environment-friendly clean alternative fuels. Due to its low NOx emission, good burning characteristics and high cetane number, dimethyl ether (DME) attracted major attention as a transportation fuel alternative. Two possible pathways have been proposed for DME production. One of these pathways is DME synthesis through conventional methanol dehydration. More recently, direct DME synthesis in a single step has attracted significant attention of researchers and fuel producers. Catalysts having two active sites are required for direct DME synthesis from synthesis gas. The aim of this work was to synthesize novel bifunctional direct DME synthesis catalysts and test their activity in a high pressure fixed bed flow reactor. Bifunctional mesoporous catalysts were synthesized by using one-pot hydrothermal synthesis, impregnation and physical mixing methods. These materials were characterized by XRD, EDS, SEM, N2 physisorption and diffuse reflectance FT-IR (DRIFTS) techniques. Characterization results of the catalysts synthesized by one-pot hydrothermal synthesis procedures in basic and acidic routes showed that pH value of the synthesis solution was highly effective on the final physical structure and chemical nature of the catalysts. Increase in the pH value promoted the incorporation of Cu, Zn and Al into the mesoporous MCM-41 structure. Also, effects of Na2CO3 addition on the catalyst structure during the hydrothermal synthesis procedure were investigated. The characterization results showed that metals were incorporated into the catalyst structure successfully. However, surface area results showed that loaded metals blocked the pores of MCM-41 and decreased the surface area of the catalysts. Effects of zirconium (Zr) metal with different weight ratios were also investigated. Results showed that Zr loading increased the surface area of the catalyst. A high pressure fixed bed flow reactor was built and the catalyst testing experiments were performed between the temperature range of 200-400&deg / C, at 50 bars. The activity results of the catalyst synthesized by impregnation method showed that no DME was formed over this catalyst / however it showed promising results for production of methanol and ethanol. Selectivity values of these alcohols were between 0.35 and 0.2. Formation of methane and CO2 indicated the occurrence of reverse dry reforming reaction. Incorporation of Zr into the catalyst structure at neutral synthesis condition caused significant activity enhancement, giving CO conversion values of about 40% at 400&deg / C. Product distribution obtained with this catalyst indicated the formation of DME, ethanol, methanol as well as CH4 and CO2. Highest DME selectivity (60%) was observed with the catalyst prepared by physical mixing of commercial methanol reforming catalyst with silicotungstic acid incorporated methanol dehydration catalyst having W/Si ratio of 0.4.

Hydrocarbon conversion and synthesis gas production are two components of the power production process that require significant development and exploration in the advanced energy arena. To remain within our current fueling infrastructure, it is imperative that an efficient and reliable mechanism to facilitate these components of the power production process is developed for automotive applications. A honeycomb monolith rhodium based catalyst has been identified as a potential fuel reformer element for use in automotive hydrocarbon fuel conversion. Using the novel and minimally invasive SpaciMS (Spatially resolved capillary inlet Mass Spectroscopy), developed at Oak Ridge National Laboratories, and an internal temperature acquisition system, the impact of fuel inlet space velocity on the operating rhodium based catalytic fuel reformer of interest was parametrically studied. In situ temperature and species profiles of the catalyst during steady state operation were produced. The data acquired through these experiments was then used to demonstrate analytic capability by conducting thermodynamic analyses on the operating fuel reformer. Experimental and analytical results can be used in development of design considerations for fuel conversion systems.

The production of synthetic fuels (synfuels) in coal–to–liquids (CTL) facilities has contributed to global warming due to the huge CO2 emissions of the process. This corresponds to inefficient carbon conversion, a problem growing in importance particularly given the limited lifespan of coal reserves. These simultaneous challenges of environmental sustainability and energy security associated with CTL facilities have been defined in earlier studies. To reduce the environmental impact and improve the carbon conversion of existing CTL facilities, this paper proposes the concept of a nuclear–assisted CTL plant where a hybrid sulphur (HyS) plant powered by 10 modules of the high temperature nuclear reactor (HTR) splits water to produce hydrogen (nuclear hydrogen) and oxygen, which are in turn utilised in the CTL plant. A synthesis gas (syngas) plant mass–analysis model described in this paper demonstrates that the water–gas shift (WGS) and combustion reactions occurring in hypothetical gasifiers contribute 67% and 33% to the CO2 emissions, respectively. The nuclear–assisted CTL plant concept that we have developed is entirely based on the elimination of the WGS reaction, and the consequent benefits are investigated. In this kind of plant, the nuclear hydrogen is mixed with the outlet stream of the Rectisol unit and the oxygen forms part of the feed to the gasifier. The significant potential benefits include a 75% reduction in CO2 emissions, a 40% reduction in the coal requirement for the gasification plant and a 50% reduction in installed syngas plant costs, all to achieve the same syngas output. In addition, we have developed a financial model for use as a strategic decision analysis (SDA) tool that compares the relative syngas manufacturing costs for conventional and nuclear–assisted syngas plants. Our model predicts that syngas manufactured in the nuclear–assisted CTL plant would cost 21% more than that produced in the conventional CTL plant when the average cost of producing nuclear hydrogen is US$3/kg H2. The model also evaluates the cost of CO2 avoided as $58/t CO2. Sensitivity analyses performed on the costing model reveal, however, that the cost of CO2 avoided is zero at a hydrogen production cost of US$2/kg H2 or at a delivered coal cost of US$128/t coal. The economic advantages of the nuclear–assisted plant are lost above the threshold cost of $100/t CO2. However, the cost of CO2 avoided in our model works out to below this threshold for the range of critical assumptions considered in the sensitivity analyses. Consequently, this paper demonstrates the practicality, feasibility and economic attractiveness of the nuclear–assisted CTL plant. / Thesis (M.Ing. (Nuclear Engineering))--North-West University, Potchefstroom Campus, 2011.

The production of synthetic fuels (synfuels) in coal–to–liquids (CTL) facilities has contributed to global warming due to the huge CO2 emissions of the process. This corresponds to inefficient carbon conversion, a problem growing in importance particularly given the limited lifespan of coal reserves. These simultaneous challenges of environmental sustainability and energy security associated with CTL facilities have been defined in earlier studies. To reduce the environmental impact and improve the carbon conversion of existing CTL facilities, this paper proposes the concept of a nuclear–assisted CTL plant where a hybrid sulphur (HyS) plant powered by 10 modules of the high temperature nuclear reactor (HTR) splits water to produce hydrogen (nuclear hydrogen) and oxygen, which are in turn utilised in the CTL plant. A synthesis gas (syngas) plant mass–analysis model described in this paper demonstrates that the water–gas shift (WGS) and combustion reactions occurring in hypothetical gasifiers contribute 67% and 33% to the CO2 emissions, respectively. The nuclear–assisted CTL plant concept that we have developed is entirely based on the elimination of the WGS reaction, and the consequent benefits are investigated. In this kind of plant, the nuclear hydrogen is mixed with the outlet stream of the Rectisol unit and the oxygen forms part of the feed to the gasifier. The significant potential benefits include a 75% reduction in CO2 emissions, a 40% reduction in the coal requirement for the gasification plant and a 50% reduction in installed syngas plant costs, all to achieve the same syngas output. In addition, we have developed a financial model for use as a strategic decision analysis (SDA) tool that compares the relative syngas manufacturing costs for conventional and nuclear–assisted syngas plants. Our model predicts that syngas manufactured in the nuclear–assisted CTL plant would cost 21% more than that produced in the conventional CTL plant when the average cost of producing nuclear hydrogen is US$3/kg H2. The model also evaluates the cost of CO2 avoided as $58/t CO2. Sensitivity analyses performed on the costing model reveal, however, that the cost of CO2 avoided is zero at a hydrogen production cost of US$2/kg H2 or at a delivered coal cost of US$128/t coal. The economic advantages of the nuclear–assisted plant are lost above the threshold cost of $100/t CO2. However, the cost of CO2 avoided in our model works out to below this threshold for the range of critical assumptions considered in the sensitivity analyses. Consequently, this paper demonstrates the practicality, feasibility and economic attractiveness of the nuclear–assisted CTL plant. / Thesis (M.Ing. (Nuclear Engineering))--North-West University, Potchefstroom Campus, 2011.