Date of Award

12-1-2017

Degree Name

Master of Science

Department

Mechanical Engineering

First Advisor

Mondal, Kanchan

Abstract

The focus of this work is to investigate the feasibility of oxygen extraction from CO2 by doped ceria in chemical looping process. In order to increase the oxygen capacity and oxygen release rates, Cerium- based oxygen carriers are doped with ZrO2. Additionally, the zirconia-doped ceria is modified by iron and copper to boost the oxygen release in the fuel reactor. It should be noted that the level of doping allows the solids to maintain the cubic fluorite structure of CeO2. The redox activity of oxygen carriers is studied in order to determine the most promising material due to the oxygen transfer capacity and methane conversion. The chemical looping dry reforming in a quartz fixed-bed reactor is carried out in two steps. In the first step, the oxygen carriers are reduced by methane through the combustion reaction. In the second step, CO2 is used for oxidation of reduced metal oxides. The obtained results at different doping levels were compared to determine the optimal oxygen carrier. The results indicate that doping ceria can boost the reactivity with methane and enhance the methane conversion during combustion reaction. CeO2 modified by Fe presents a progress in both oxygen release and uptake with an increase in oxygen capacity of metal oxide. However, zirconia and copper ceria show different effect on reduction and oxidation. This means that zirconia doped ceria results in an increase in oxygen release during reduction and decrease in oxygen uptake during oxidation with CO2. In contrast, addition of copper to ceria metal oxides shows a negative effect on oxygen release, while it enhances the ability of oxygen uptake. Out of all mixed cerium oxides investigated in this study, cerium oxide containing 10% mole iron is determined as the most promising oxygen carrier for CLDR due to the methane conversion, facilitating oxygen release, increasing the level of reduction and improving the oxidation uptake of the metal oxide in the reaction with CO2.

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