Pressurized Chemical Looping Combustion of Natural Gas with Ilmenite for SAGD Application: An Oxidation Kinetic Study and Preliminary Air Reactor Model

Abstract

To prevent the global surface temperature from increasing past the 2 oC target, it is necessary to address CO2 emissions from small point sources. Within Canada’s heavy oil industry, SAGD facilities use natural gas combustion to produce the large amounts of steam required for the process, which produces approximately 0.5-2 Mtonnes of CO2 per annum. A suitable technology for CO2 mitigation from a SAGD facility is Pressurized Chemical Looping Combustion. PCLC is an oxy-combustion, carbon capture technology with a relatively low predicted energy penalty of 3-4%. The process requires a dual, interconnected fluidized bed reactor system with circulating solids. Natural gas is converted in the fuel reactor via a solid metal oxide, which is then circulated to the air reactor for reoxidation with air. As the cost of air compression is significant, the economical feasibility of the process is reliant on air reactor performance. The objective of this study is to investigate the oxidation reaction and derive a kinetic model for reactor design and performance assessment purposes. Ilmenite ore was chosen as the metal oxide, as it is low cost and has desirable oxygen transport properties for PCLC. Pressurized TGA tests were conducted to study the effects of oxygen concentration, temperature and pressure on the rate of the oxidation reaction. The total pressure was varied from 1-16 bara at 900 oC with air. The oxygen concentration was varied from 2.5-21 vol%, and the temperature from 800-1000 oC at 8 bar. Temperatures below 850 oC resulted in segregation of the Fe and Ti phase in the ilmenite ore, leading to a reduction in the overall oxygen carrying capacity. Crack formation was observed at higher oxygen partial pressures, resulting in increased surface area for reaction and a fast reaction rate. At lower oxygen partial pressures, a solid-state diffusion controlled regime was observed due to the absence of fissures. A dual mechanistic oxidation kinetic model was derived at 8 bar, with 2nd order random nucleation dominating at lower conversions, and Jander’s solid state diffusion model dominating at higher conversions. The transition from the nucleation and growth to the diffusion-controlled portion occurred at higher conversions with higher oxygen partial pressure. The activation energy was 16.6 kJ/mol and 48.7 kJ/mol while the order of reaction with respect to oxygen was 0.3 and 1.3 for respectively the nucleation and growth, and diffusion-controlled regimes. A preliminary air reactor model is constructed as a turbulent bed. The turbulent bed is modelled as an axial dispersion reactor for a basic performance assessment.