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SMSI effects on CO adsorption and hydrogenation on Pt catalysis

Journal Article · · J. Catal.; (United States)
OSTI ID:6264472
Infrared spectroscopy has been employed to characterize adsorbed CO species under steady-state reaction conditions in the presence of H/sub 2/ and also under equilibrium adsorption conditions in the presence of He. During reaction, kinetic data were obtained simultaneously with ir spectra using a special ir reactor cell. Turnover frequencies on Pt were found to vary more than 100-fold as the support material varied, and the activity ranking of these catalysts was: Pt/TiO/sub 2/ (SMSI) > Pt/TiO/sub 2/ (LT) greater than or equal to Pt/eta-Al/sub 2/O/sub 3/ approx. = Pt/SiO/sub 2/-Al/sub 2/O/sub 3/ > Pt/SiO/sub 2/. Two principal ir bands were observed on Pt - a high-frequency band between 2050 and 2080 cm/sup -1/ and a low-frequency band between 1780 and 1860 cm/sup -1/. Except for TiO/sub 2/-supported Pt, very similar behavior was observed, i.e., intense ir bands occurred which were nearly insensitive to temperature and the presence of H/sub 2/, and these catalysts exhibited strong bands under reaction conditions. In contrast, the Pt/TiO/sub 2/ (SMSI) catalyst showed almost no ir-detectable CO during reaction and, even more surprising, CO band intensities were also markedly reduced at 300 K by the presence of H/sub 2/. No obvious correlation was found between detectable CO species and specific activity; however, this study strongly infers that only a very small fraction of surface Pt atoms constitute active sites, and the higher activity occurring on the SMSI Pt/TiO/sub 2/ catalyst is attributed to a weakened CO-metal bond resulting in more competitive H/sub 2/ chemisorption and higher surface concentrations of hydrogen under reaction conditions.
Research Organization:
Pennsylvania State Univ., University Park
DOE Contract Number:
AC02-77ER04463
OSTI ID:
6264472
Journal Information:
J. Catal.; (United States), Journal Name: J. Catal.; (United States) Vol. 79:1; ISSN JCTLA
Country of Publication:
United States
Language:
English