Chemical looping combustion (CLC) is a technique for separating pure carbon dioxide from the combustion of fuels. The oxygen to burn the fuel comes from the lattice oxygen contained in solid particles of an inorganic oxide (the ‘oxygen carrier’), instead of from oxygen in the air. Thus only CO2 and water leave the combustor, or fuel reactor. Next, the water is condensed, leaving pure CO2. The oxygen carrier is regenerated by oxidising it in air in a second reactor, called the air reactor. Accordingly, a stream of pure carbon dioxide can be produced, uncontaminated with gases such as nitrogen, normally present when the fuel burns in air. This intrinsic separation with CLC enables CO2 to be separated more efficiently than with other techniques, such as post-combustion scrubbing of carbon dioxide from stack gases with amine-based solvents.

The design of a CLC system and its performance within an electricity system represents a multi-scale problem, ranging from the behaviour of single particles of oxygen carrier within a reactor to how a CLC-based power plant would perform in an electricity grid. To date, these scales have been studied in isolation, with little regard for the vital interactions and dependences amongst them. This Dissertation addresses this problem by considering CLC holistically for the first time, using a multi-scale approach.

A stochastic model was developed, combining the particle-and reactor-scales of CLC. It included an appropriate particle model and can be coupled to a detailed reactor model. The combination represented a significant change from existing approaches, uniquely accounting for all the important factors affecting the assemblage of particles performing in the CLC reactors. It was used to determine the regimes of operation in which CLC is sensitive to factors such as the manner in which the particles are reacting, the residence time distribution of particles in the two reactors, the particle size distribution and the reaction history of particles. To demonstrate that the approach could simulate specific configurations of CLC, as well as a general system, the model was compared with results from experiments in which CLC with methane was conducted in a laboratory-scale circulating fluidised bed.

The long-term performance of oxygen carrier materials is important, because, in an industrial process, they would be expected to function satisfactorily for many thousands of hours of operation. Long-term experiments were conducted to evaluate the resistance of different oxygen carrier materials to physical and chemical attrition. The evolution of their chemical kinetics was also determined. The results were used to evaluate the impact of different oxygen carrier materials in a fuel reactor at industrial-scale.

Finally, a theoretical approach was developed to simulate how a fleet of CLC-based power plants would perform within the UK’s national grid. By understanding how different parameters such as capital cost, operating cost and measures of efficiency, compared with other methods of generation offering carbon reduction, desirable design modifications and needs for improvement for CLC were identified by utilising the theoretical and experimental work conducted at the particle- and reactor-scales.