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In situ XPS measurements of Reforming Catalysts


EMSL Project ID
6300

Abstract

This proposal is to perform in situ X-ray photoelectron spectroscopy (XPS) characterization of some reforming (powder) catalysts. We, at Penn State University, under the supervision of Prof.Chunshan Song, is working on the development of catalysts for the reforming of methanol, ethanol, liquid hydrocarbons such as jet fuel to produce hydrogen for fuel cell applications. We are also working on the development of new generation catalysts for low-temperature water-gas shift reaction. Our group has been developing bi-metallic/multi-metallic catalysts composed of base metals/noble metals supported on different supports such as ceria, alumina and zirconia. Since most of these catalysts are reduced before the reaction, we are interested to characterize the reduced samples in situ by XPS in order to identify the nature of active species and their surface concentrations. We are interested in measuring the XPS of about 20 reforming catalysts employed in the reforming of methanol/ethanol/jet fuel, unreduced and reduced in situ. We would like to reduce the catalyst samples in situ in hydrogen/argon mixture for 3-5 h in the temperature range 300 to 500 degree C. We would like to measure the kinetic energy/binding energy of metals/metal ions in the core level regions. If necessary, we would also like to measure the binding energy in the valence band regions as well in order to investigate the synergistic effect of multi-metals on the binding energy at the Fermi level. The results of these experiments would be very helpful to understand the nature of active sites on the surface of the reforming catalysts. We have been evaluating the catalytic performance of these new catalysts in the reforming reaction at Penn State. The XPS data/results would be very helpful to understand and correlate the catalytic performance (conversion/selectivity) with the nature of active species and hence to establish structure-activity relationship. The results of the work will be discussed thoroughly with the PNNL scientists responsible for the work, manuscripts will be drafted and published in well-reputed international journals. The PNNL scientists will be included as author(s) and the EMSL will be gratefully acknowledged for providing instrumental facility. The interest in the catalytic reforming of natural gas, methanol, ethanol, biomass and liquid hydrocarbons to produce hydrogen is increasing in recent years in order to integrate the catalytic reformers with fuel cells for power generation in automobiles and stationary power plants. Fundamental understanding of the nature of active sites in the reforming and water-gas shift catalysts will be very useful to develop a highly active catalyst. Thus, the outcome of this work will be great contribution to the scientific community.

Project Details

Project type
Exploratory Research
Start Date
2004-02-01
End Date
2006-03-23
Status
Closed

Team

Principal Investigator

Velu Subramani
Institution
Research Triangle Institute

Team Members

Chunshan Song
Institution
Pennsylvania State University

Related Publications

Adsorptive Removal of Organic Sulfur compounds from jet fuel over K-exchanged NiY zeolites prepared by impregnation and ion exchange. Ind.Eng.Chem. Res. 2005, 44, 5740
Fox E, S Velu, MH Engelhard, YH Chin, JT Miller, J Kropf, and C Song. 2008. "Characterization of CeO2-Supported Cu-Pd Bimetallic Catalyst for the Oxygen-Assisted Water-Gas Shift Reaction." Journal of Catalysis 260(2):358-370
Kugai J, V Subramani, C Song, MH Engelhard, and Y Chin. 2006. "Effects of nanocrystalline CeO2 supports on the properties and performance of Ni?Rh bimetallic catalyst for oxidative steam reforming of ethanol." Journal of Catalysis 238(2):430-440.