Abstract
The utility of surface-enhanced Raman spectroscopy (SERS) as an in situ adsorbate probe of heterogeneous catalytic systems at high gas pressures (here up to 1 atm) in conjunction with mass spectrometry (MS) is demonstrated for reactions on transition-metal catalysts, at temperatures up to 500 °C. This simultaneous SERS−MS approach enables the relationships between the formation of specific adsorbed species (as sensed by SERS) and reaction products (as detected by MS) to be explored on a common (≈1 s) time scale. The low-frequency (<1000 cm-1) spectral region, where metal−adsorbate vibrations are located, is especially informative. The environmentally important reactions of NO reduction by CO or H2 and the oxidation of methanol on transition metals (Rh, Pd, Pt) are considered here. The possible mechanistic significance of surface oxide formation observed during such ambient-pressure catalytic reactions is also discussed.
Published Version
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