High Pressure Catalytic Processes Studied by Infrared-Visible SumFrequency Generation
The recent development of infrared-visible sum frequency generation (SFG), a surface-specific vibrational spectroscopy, has helped bridge the pressure gap between studies of heterogeneous catalysis under high vacuum and atmospheric pressure. This is achieved by in situ monitoring of surface species at high pressure via their SFG vibrational spectra and correlating the results with the simultaneously measured reaction rate using gas chromatography. Examples of systems studied include olefin hydrogenation and carbon monoxide oxidation over the (111) crystalline face of platinum. In these examples, the studies succeed in revealing the molecular details of the surface reactions. Identification of key intermediates and their concentrations has made it possible for the first time to calculate turn over rates per active surface species rather than just per exposed surface metal atom. In all cases, the key intermediate of the reaction is not detectable on the surface in UHV under similar temperatures.
- Research Organization:
- Ernest Orlando Lawrence Berkeley NationalLaboratory, Berkeley, CA (US)
- Sponsoring Organization:
- USDOE Director, Office of Energy Research
- DOE Contract Number:
- AC02-05CH11231
- OSTI ID:
- 899775
- Report Number(s):
- LBNL--40657
- Journal Information:
- Journal of Molecular Catalysis A: Chemical, Journal Name: Journal of Molecular Catalysis A: Chemical Journal Issue: 1 Vol. 131; ISSN JMCCF2
- Country of Publication:
- United States
- Language:
- English
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Molecular studies of catalytic reactions on crystal surfaces at high pressures and high temperatures by infrared-visible sum frequency generation (SFG) surface vibrational spectroscopy
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