In situ TPR XANES study of the partial oxidation of methane using a Ni-substituted hexaaluminate catalyst

FUEL 216

Edwin L. Kugler, edwin.kugler@mail.wvu.edu1, Todd H. Gardner, todd.gardner@netl.doe.gov2, Andrew Campos, acampo2@lsu.edu3, Jason Hissam, jhissam@mix.wvu.edu1, James J. Spivey, jjspivey@lsu.edu3, and Amitava D. Roy, reroy@lsu.edu4. (1) Department of Chemical Engineering, West Virginia University, Morgantown, WV 26506-6102, (2) National Energy Technology Laboratory, U.S. Department of Energy, 3610 Collins Ferry Road, Morgantown, WV 26507-0880, (3) Dept. of Chemical Engineering, Louisiana State University, S. Stadium Drive, Baton Rouge, LA 70803, (4) Center for Advanced Microstructures and Devices, Louisiana State University, 6980 Jefferson Highway, Louisiana State University, Baton Rouge, LA 70806
Metallic Ni formation near the mirror cation site, Ba in this study, is believed to cause the partial oxidation activity observed in Ni-substituted hexaaluminate catalysts. The BaNi1.0Al11.6O19-d catalyst was prepared by coprecipitation with nitrate salt precursors; following the coprecipitation procedure, the catalyst was calcined at 1400°C to create the hexaaluminate structure. TPR XANES in fluorescence was used to probe the local structure of the BaNi1.0Al11.6O19-d catalyst to determine whether metallic nickel forms at different temperatures: 825°C, 875°C, 925°C. The XANES results indicate that the Ni in the hexaaluminate catalyst only reduces if the temperature is maintained at 925°C. Once the metallic state is formed, the oxidation state is stable; even in the POX environment. Future work using a theoretical approach to the XANES data using FEFF 8.4 gives information on the interactions between Ni and Ba, which will be used to further optimize the catalyst.
 

Ultraclean Transportation Fuels
1:30 PM-5:30 PM, Wednesday, April 9, 2008 Morial Convention Center -- Rm. 239, Oral

Division of Fuel Chemistry

The 235th ACS National Meeting, New Orleans, LA, April 6-10, 2008