It is proposed that an integrated ammonia-PEM fuel cell could unlock the potential of ammonia to act as a high capacity chemical hydrogen storage vector and enable renewable energy to be delivered eectively to road transport applications. Catalysts are developed for low temperature ammonia decomposition with activity from 450 K (ruthenium and cesium on graphitised carbon nanotubes). Results strongly suggest that the cesium is present on the surface and close proximity to ruthenium nanoparticles and that it produces activity in ruthenium by donation of electrons. The activity of sustainable cobalt for ammonia decomposition is shown to be a function of particle size and is more active on microporous carbon supports compared to mesoporous ones. Unlike ruthenium, activity for cobalt was not inuenced by the degree of surface graphitic nature and cobalt supported on microporous carbon approached the activity of ruthenium on the same support. In accordance with the sustainable objectives of this thesis, a case-study on the sustainability of ammonia as a sustainable hydrogen storage vector was undertaken. In this scheme, hydrogen produced from renewable electricity by electrolysis is con- verted to ammonia by the Haber-Bosch process and then converted back to deliver pure hydrogen at the point of use. The energy eciency and carbon footprint fell short of targets set by the US Department of Energy and the UK Department for Transport, the biggest impact was the production of hydrogen by electrolysis and not the Haber-Bosch process which accounts for only 9 % of total energy losses. To assess the feasibility of the ammonia-PEM fuel cell, a conceptual design was un- dertaken to quantify the palladium membrane size and catalyst quantity required for a typical road transport vehicle. The predicted quantity of palladium was excessive and future work must consider improvements to membrane technology.

<p>  </p> <p>With economies shifting towards net-zero carbon emissions, there is an increased interest in carbon-free energy carriers. Hydrogen is a potential carbon-free energy source. However, it poses several production, infrastructural, and safety challenges. Ammonia blends have been identified as a potential hydrogen carrier and fuel for gas turbine combustion. Partially cracked ammonia mixtures consist of large quantities of hydrogen that help overcome the disadvantages of pure ammonia combustion. The presence of nitrogen in the fuel blends leads to increased NO_x emissions, and therefore lean premixed combustion is necessary to curb these emissions. Understanding the flame features, precursors, and dynamics of blowout of such blends due to lean conditions is essential for stable operation, lean blowout prediction, and control. </p> <p><br></p> <p>In this study, high-fidelity large eddy simulations for turbulent premixed ammonia/hydrogen/nitrogen-air flames in an axisymmetric, unconfined, bluff-body stabilized burner are performed to gain insights into lean blowout dynamics. Partially cracked ammonia (40% NH₃, 45% H₂, and 15% N₂, by volume) is chosen as fuel since its laminar burning velocity is comparable to CH4-air mixtures. A finite rate chemistry model with a detailed chemical kinetic mechanism (36 species and 247 reactions) is utilized to capture characteristics of various species during blowout. A comprehensive study of the flow field and flame structure for a weakly stable burning at an equivalence ratio of 0.5 near the blowout limit is presented. Further, the effects of blowout on the heat release rate, vorticity, distribution of major species, and ignition radicals are studied at four time instances at blowout velocity of 70 m/s. Since limited data is available on turbulent premixed combustion of partially cracked ammonia, such studies are essential in understanding flame behavior and uncertainties with regard to blowout.</p>

The performance of solid oxide fuel cells (SOFCs) at the cell and system levels is studied using computer simulation. At the cell level, a new model combining the cell micro and macro models is developed. Using this model, the microstructural variables of porous composite electrodes can be linked to the cell performance. In this approach, the electrochemical performance of porous composite electrodes is predicted using a micro-model. In the micro-model, the random-packing sphere method is used to estimate the microstructural properties of porous composite electrodes from the independent microstructural variables. These variables are the electrode porosity, thickness, particle size ratio, and size and volume fraction of electron-conducting particles. Then, the complex interdependency among the multi-component mass transport, electron and ion transports, and the electrochemical and chemical reactions in the microstructure of electrodes is taken into account to predict the electrochemical performance of electrodes. The temperature distribution in the solid structure of the cell and the temperature and species partial pressure distributions in the bulk fuel and air streams are predicted using the cell macro-model. In the macro-model, the energy transport is considered for the cell solid structure and the mass and energy transports are considered for the fuel and air streams. To demonstrate the application of the cell level model developed, entitled the combined micro- and micro-model, several anode-supported co-flow planar cells with a range of microstructures of porous composite electrodes are simulated. The mean total polarization resistance, the mean total power density, and the temperature distribution in the cells are predicted. The results of this study reveal that there is an optimum value for most of the microstructural variables of the electrodes at which the mean total polarization resistance of the cell is minimized. There is also an optimum value for most of the microstructural variables of the electrodes at which the mean total power density of the cell is maximized. The microstructure of porous composite electrodes also plays a significant role in the mean temperature, the temperature difference between the hottest and coldest spots, and the maximum temperature gradient in the solid structure of the cell. Overall, using the combined micro- and micro-model, an appropriate microstructure for porous composite electrodes to enhance the cell performance can be designed. At the system level, the full load operation of two SOFC systems is studied. To model these systems, the basic cell model is used for SOFCs at the cell level, the repeated-cell stack model is used for SOFCs at the stack level, and the thermodynamic model is used for the balance of plant components of the system. In addition to these models, a carbon deposition model based on the thermodynamic equilibrium assumption is employed. For the system level model, the first SOFC system considered is a combined heat and power (CHP) system that operates with biogas fuel. The performance of this system at three different configurations is evaluated. These configurations are different in the fuel processing method to prevent carbon deposition on the anode catalyst. The fuel processing methods considered in these configurations are the anode gas recirculation (AGR), steam reforming (SR), and partial oxidation reformer (POX) methods. The application of this system is studied for operation in a wastewater treatment plant (WWTP) and in single-family detached dwellings. The evaluation of this system for operation in a WWTP indicates that if the entire biogas produced in the WWTP is used in the system with AGR or SR fuel processors, the electric power and heat required to operate the plant can be completely supplied and the extra electric power generated can be sold to the electrical grid. The evaluation of this system for operation in single-family detached dwellings indicates that, depending on the size, location, and building type and design, this system with all configurations studied is suitable to provide the domestic hot water and electric power demands. The second SOFC system is a novel portable electric power generation system that operates with liquid ammonia fuel. Size, simplicity, and high electrical efficiency are the main advantages of this environmentally friendly system. Using a sensitivity analysis, the effects of the cell voltage at several fuel utilization ratios on the number of cells required for the SOFC stack, system efficiency and voltage, and excess air required for thermal management of the SOFC stack are studied.

The performance of solid oxide fuel cells (SOFCs) at the cell and system levels is studied using computer simulation. At the cell level, a new model combining the cell micro and macro models is developed. Using this model, the microstructural variables of porous composite electrodes can be linked to the cell performance. In this approach, the electrochemical performance of porous composite electrodes is predicted using a micro-model. In the micro-model, the random-packing sphere method is used to estimate the microstructural properties of porous composite electrodes from the independent microstructural variables. These variables are the electrode porosity, thickness, particle size ratio, and size and volume fraction of electron-conducting particles. Then, the complex interdependency among the multi-component mass transport, electron and ion transports, and the electrochemical and chemical reactions in the microstructure of electrodes is taken into account to predict the electrochemical performance of electrodes. The temperature distribution in the solid structure of the cell and the temperature and species partial pressure distributions in the bulk fuel and air streams are predicted using the cell macro-model. In the macro-model, the energy transport is considered for the cell solid structure and the mass and energy transports are considered for the fuel and air streams. To demonstrate the application of the cell level model developed, entitled the combined micro- and micro-model, several anode-supported co-flow planar cells with a range of microstructures of porous composite electrodes are simulated. The mean total polarization resistance, the mean total power density, and the temperature distribution in the cells are predicted. The results of this study reveal that there is an optimum value for most of the microstructural variables of the electrodes at which the mean total polarization resistance of the cell is minimized. There is also an optimum value for most of the microstructural variables of the electrodes at which the mean total power density of the cell is maximized. The microstructure of porous composite electrodes also plays a significant role in the mean temperature, the temperature difference between the hottest and coldest spots, and the maximum temperature gradient in the solid structure of the cell. Overall, using the combined micro- and micro-model, an appropriate microstructure for porous composite electrodes to enhance the cell performance can be designed. At the system level, the full load operation of two SOFC systems is studied. To model these systems, the basic cell model is used for SOFCs at the cell level, the repeated-cell stack model is used for SOFCs at the stack level, and the thermodynamic model is used for the balance of plant components of the system. In addition to these models, a carbon deposition model based on the thermodynamic equilibrium assumption is employed. For the system level model, the first SOFC system considered is a combined heat and power (CHP) system that operates with biogas fuel. The performance of this system at three different configurations is evaluated. These configurations are different in the fuel processing method to prevent carbon deposition on the anode catalyst. The fuel processing methods considered in these configurations are the anode gas recirculation (AGR), steam reforming (SR), and partial oxidation reformer (POX) methods. The application of this system is studied for operation in a wastewater treatment plant (WWTP) and in single-family detached dwellings. The evaluation of this system for operation in a WWTP indicates that if the entire biogas produced in the WWTP is used in the system with AGR or SR fuel processors, the electric power and heat required to operate the plant can be completely supplied and the extra electric power generated can be sold to the electrical grid. The evaluation of this system for operation in single-family detached dwellings indicates that, depending on the size, location, and building type and design, this system with all configurations studied is suitable to provide the domestic hot water and electric power demands. The second SOFC system is a novel portable electric power generation system that operates with liquid ammonia fuel. Size, simplicity, and high electrical efficiency are the main advantages of this environmentally friendly system. Using a sensitivity analysis, the effects of the cell voltage at several fuel utilization ratios on the number of cells required for the SOFC stack, system efficiency and voltage, and excess air required for thermal management of the SOFC stack are studied.