Graduation Year

2019

Document Type

Thesis

Degree

M.S.M.S.E.

Degree Name

MS in Materials Science and Engineering (M.S.M.S.E)

Degree Granting Department

Chemical Engineering

Major Professor

Venkat Bhethanabotla, Ph.D.

Co-Major Professor

John Kuhn, Ph.D.

Committee Member

Scott Campbell, Ph.D.

Keywords

catalyst, CO2 recycling, greenhouse gas, low temperature conversion, reverse water-gas shift chemical looping

Abstract

As the greenhouse gas effect becomes more serious, it is important to find an effective way to reduce carbon dioxide emissions and/or convert it to value-added products. Based on the catalytic requirements, convert CO2 to CO using perovskite-type oxides which are suitable for reverse water-gas shift chemical looping (RWGS-CL). The resulting carbon monoxide can be subsequently used for chemical energy storage in the form of hydrocarbon-based fuels and chemicals. This research focuses on the synthesis of the LaxBa1-xFeyAl1-yO3 perovskite-type oxides, which can form oxygen vacancies, or active sites for CO2 conversion.

Multiple measurement methods were using for testing synthesized catalysts. Temperature-programmed reduction (TPR) and temperature-programmed oxidation (TPO) experiments were performed to identify reaction temperatures and redox properties of the materials. Surface areas were measured, and X-ray diffraction was utilized to identify the crystal structure.

La0.25Ba0.75FeO3 and La0.5Ba0.5FeO3 were showed an appreciate conversion property, and comparison was made between these two compositions. Results showed La0.25Ba0.75FeO3 can converted more CO and La0.5Ba0.5FeO3 made conversion in high stability.

Components of A site and B site element were analyzed based on characterization results, which showed lanthanum can increase catalyst stability, barium can increase CO yield, iron showed a better property as a B site component than aluminum.

In summary, this research based on serious CO2 emission problem in the world, synthesized LaxBa1-xFeyAl1-yO3, nine perovskite oxide catalysts, to convert wasted CO2 to CO. Comparison was made with other perovskite-type catalysts for RWGS-CL, the results showed the two samples were advantageous on lower conversion temperature of 500°C.

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