Steam Reforming of Ethanol over Pt/ceria with Co-Fed Hydrogen
Metal/ceria catalysts are receiving great interest for reactions involving steam conversion, including CO for low-temperature water-gas shift, and the conversion of chemical carriers of hydrogen, among them methanol, and ethanol. The mechanism by which ROH model reagents are activated on the surface of the Pt/partially reduced ceria catalyst was explored using a combination of reaction testing and infrared spectroscopy. In this particular investigation, the activation and turnover of ethanol were explored and compared with previous investigations of methanol steam reforming and low-temperature water-gas shift under H2-rich conditions, where the surface of ceria is in a partially reduced state. Under these conditions, activation of ethanol was found to proceed by dissociative adsorption at reduced defect sites on ceria (i.e., Ce surface atoms in the Ce3+ oxidation state), yielding an adsorbed type II ethoxy species and an adsorbed H species, the latter identified to be a type II bridging OH group. In the presence of steam, the ethoxy species rapidly undergoes molecular transformation to an adsorbed acetate intermediate by oxidative dehydrogenation. This is analogous to the conversion of type II methoxy species to formate observed in previous investigations of methanol steam reforming. In addition, although formate then decomposes in steam to CO2 and H2 during methanol steam reforming, in an analogous pathway for ethanol steam reforming, the acetate intermediate decomposes in steam to CO2 and CH4. Therefore, further H2 production requires energy-intensive activation of CH4, which is not required for methanol conversion over Pt/ceria.
- Research Organization:
- Brookhaven National Laboratory (BNL) National Synchrotron Light Source
- Sponsoring Organization:
- Doe - Office Of Science
- DOE Contract Number:
- AC02-98CH10886
- OSTI ID:
- 959707
- Report Number(s):
- BNL--82693-2009-JA
- Journal Information:
- Journal of Catalysis, Journal Name: Journal of Catalysis Vol. 245; ISSN 0021-9517; ISSN JCTLA5
- Country of Publication:
- United States
- Language:
- English
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