Isotopic transient kinetic analysis of CO hydrogenation on Cu-modified Ru/SiO{sub 2}
- Univ. of Pittsburgh, PA (United States)
The effect of Cu decoration of Ru/SiO{sub 2} on CO hydrogenation at 1 atm has been studied by isotopic transient kinetics analysis for catalysts having Cu/Ru atomic ratios of 0-0.5. The abundances, coverages, and lifetimes of surface intermediates of the reaction were measured under reaction conditions using isotopic transient kinetic analysis. The effects of temperature and partial pressure of H{sub 2} on these surface reaction parameters were also investigated. Activity distribution analysis showed that there were primarily two kinds of active methanation sites/intermediates (related to pools {alpha} and {beta}) as has previously been noted by a number of researchers. Cu preferentially blocked {alpha}-type sites. The surface abundance for pool {alpha} monotonically decreased with Cu loading while that for pool {beta} only decreased for Cu/Ru>0.1. Some additional low activity sites for methanation may have been generated with Cu addition due to (a) the spillover of H and CH{sub x} from Ru to Cu permitting reaction to occur on the Cu, or (b) the creation of {beta}-type sites at the Ru-Cu interfaces. The surface abundance of CO measured during the reaction suggests that (a) there was significant spillover of CO from Ru to Cu, and (b) Cu not only blocked the Ru surface but may have possibly caused some reconstruction of it. The surface abundance of intermediates was independent of H{sub 2} partial pressure in the range 18-55 kPa for all the catalysts. 30 refs., 15 figs., 9 tabs.
- OSTI ID:
- 263704
- Journal Information:
- Journal of Catalysis, Journal Name: Journal of Catalysis Journal Issue: 2 Vol. 158; ISSN JCTLA5; ISSN 0021-9517
- Country of Publication:
- United States
- Language:
- English
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