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In Situ Real-Time Studies of Heterogeneous Catalytic Mechanisms at Ambient Pressures As Probed by Surface-Enhanced Raman and Mass Spectroscopies
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文摘
The utility of surface-enhanced Raman spectroscopy (SERS) as an insitu adsorbate probe ofheterogeneous catalytic systems at high gas pressures (here up to 1atm) in conjunction withmass spectrometry (MS) is demonstrated for reactions ontransition-metal catalysts, attemperatures up to 500 C. This simultaneous SERS-MS approachenables the relationshipsbetween 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 (<1000cm-1) spectral region, wheremetal-adsorbate vibrations are located, is especiallyinformative.The environmentally important reactions of NO reduction by CO orH2 and the oxidation ofmethanol on transition metals (Rh, Pd, Pt) are considered here.The possible mechanisticsignificance of surface oxide formation observed during suchambient-pressure catalytic reactionsis also discussed.

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