Year of Publication

2013

Degree Name

Doctor of Philosophy (PhD)

Document Type

Doctoral Dissertation

College

Engineering

Department

Mechanical Engineering

First Advisor

Dr. Kozo Saito

Abstract

According to IPCC reports, the greenhouse gas CO2 is responsible for global climate change. Studies show that CO2 concentration reached a level of 400 ppm in 2013, or 40 % above pre-industrial levels. The contribution of CO2 from industrial activity to increasing global CO2 concentrations is widely accepted and points to the need to reduce the emission of this greenhouse gas.One possible combustion technology that shows promise for reducing CO2 emissions is chemical looping combustion (CLC). It is an oxy-fuel technology, but has the advantages of in situ oxygen separation, low NOx emissions and low cost of CO2 emission abatement; it entails the use of an oxygen carrier (OC) to provide oxygen for combusting fuels.

OC development is an important task in CLC. Iron based OCs have attracted most research attention in recent years, mainly due to their inexpensive and non-toxic nature. Bi-metal oxide OCs usually impart better CLC performance than mono-metal oxide OCs, one example of which is the introduction of CeO2 as a partially reducible material capable of generating oxygen vacancies that lead to oxygen storage and transfer. In this study, CeO2 was used as an additive to a Fe2O3-based OC and its effect on physical properties, such as morphology, surface area and mechanical strength, was analyzed in detail. The reactivity of OCs is studied using TGA-MS and a bench scale CLC setup. The results show that the reduction reaction at the surface is independent of whether CeO2 is present or not, but after the surface oxygen had been consumed, the OC with CeO2 provided faster oxygen transfer rates from the bulk to the surface to produce better average reaction rates. The OCs after reduction and oxidation were analyzed using XRD and Raman spectroscopy; based on these analytical data, a model for the promoting role of CeO2 is discussed. Furthermore, the reaction kinetics of the OCs were also studied using shrinking core model, the kinetics parameters were obtained and compared.

Scale-up of laboratory-scale CLC reactors is another important task necessary to develop an understanding of the potential and efficiencies of CLC. In this study, scaling laws were used as a guide to design and then build two different-sized CLC reactors. Testing of the reactors involved a focus on chemical similarities. Comparisons of the performance of both reactors showed good consistency, thereby validating the scale modeling method and the scale laws for CLC reactors.

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