The use of a spray-pyrolysis method is studied for the continuous synthesis of refractory oxide reforming catalyst for the conversion of hydrocarbon fuels to H2 and CO at 900°C. Nickeland rhodium-doped zirconate pyrochlore materials with the formulas La1.89Ni2.81Y0.25Ca0.11Zr1.47 and La1.89Rh1.09Y0.25Ca0.11Zr1.641 were synthesized using the spray pyrolysis method. Both Pechini and glycine-nitrate precursor solutions were used in order to control the particle morphology, crystallinity, and surface area of the catalyst powder. Samples synthesized by the Pechini solution required post-synthesis heat treatment to 1000 °C for 2 hours to form the fullycrystalline pyrochlore phase. Both the Ni-and Rh-doped compositions formed by the spraypyrolysis method performed as reported elsewhere for powder produced by solid-state and Pechini bulk methods. The use of the glycine-nitrate precursor solution in the spray-pyrolysis resulted in the formation of fully crystalline pyrochlore catalyst for the Ni-doped composition without any additional high temperature treatment. The Rh-doped catalysts synthesized from the glycine-nitrate precursor did not form a fully crystalline material directly from the spraypyrolysis process, but required a further thermal treatment to 800 °C for 8 hours to transform the powder and burn-off excess carbon remaining from the synthesis process. Rapid catalyst aging tests for the Rh-doped catalysts synthesized by spray-pyrolysis (using either the Pechini and glycine-nitrate precursor solutions) produced stable and active catalysts achieving equilibrium hydrogen yield of 90% for 15 hours. To conclude, the work showed that through proper chemical design of the precursor system, a high surface area, chemically active, and stable zirconate pyrochlore catalyst could be synthesized efficiently by the spray-pyrolysis method developed. iii Acknowledgements This work would not have been possible without the support and guidance of my advisor Dr. Edward M. Sabolsky. The lab skills I have developed under his tutelage during the last 5 years are invaluable, and I thank him for his patience in completing this work. I would also like to thank Dr. Dushyant Shekhawat at NETL for his advice and making equipment available for my use, without which my thesis would not yet be complete. Kathy Sabolsky has been of great help for all my years spent as both an undergraduate and graduate researcher. I am grateful to Dr. Mark Smith for his time, help and friendship. Donald Floyd was of great help in characterization of my samples, and without his work with the reforming reactors I would not be able to complete this work. I would also like to thank Dave Berry, Dan Haynes, and Dr. Devendra Pakhare for their advice and time during the project. The support of my mother Terri Yancey is essential to any of my successes, and the encouragement from my brother Jeffrey Yancey has been important in all of my endeavors. Without the "unique" problem solving skills imparted in me by my father Brent Yancey and grandfather Gerald Yancey I would ...