Date of Completion

1-9-2015

Embargo Period

7-6-2015

Keywords

Chemical-looping, Carbon Capture, Kinetics, Reactor modeling

Major Advisor

George M. Bollas

Associate Advisor

Ioulia Valla

Associate Advisor

Steven Suib

Associate Advisor

Brian Willis

Associate Advisor

Ranjan Srivastava

Field of Study

Chemical Engineering

Degree

Doctor of Philosophy

Open Access

Campus Access

Abstract

Chemical-looping combustion (CLC) is a method for the oxidation of hydrocarbons with in-situ O2 separation, resulting in energetically inexpensive CO2 sequestration. The basic concept of the process involves using a metal oxide as an oxygen carrier (OC) to transfer oxygen from an Oxidizer reactor to a Reducer reactor, where the hydrocarbons are oxidized by the lattice oxygen of the OC. The reduced oxygen carrier is then re-oxidized in the Oxidizer. Chemical-looping with oxygen uncoupling (CLOU) is very similar to normal CLC, with the major difference that the process employs certain metal oxides as oxygen carriers. CLOU takes advantage of the exothermic and spontaneous splitting of some metal oxides at high temperature, resulting in an overall thermodynamically favorable process for the transport of oxygen between the two reactors.

The aim of this dissertation is to provide insights to the feasibility and efficiency of CLC, by closing the gap between simulation and experimentation in bench- and pilot-scale chemical-looping processes. The key ideas in this dissertation are to combine experimentation and dynamic simulation, understand the current experimental procedures for chemical-looping, and expand the laboratory finding to conceptual commercial systems.

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