A transient kinetic study of nickel-catalyzed methanation: Final report

Technical Report · Tue Nov 01 04:00:00 EST 1988

OSTI ID:6566396

Hoost, T E; Goodwin, Jr, J G

The results of this study are in two major parts. In Part I the use of steady-state isotopic transients of multiple elements (C, H, and O) under actual methanation reaction conditions has permitted an assessment of the reactivity of water on a Ni powder catalyst. It was concluded based on the addition of isotopic water that oxygen, once reacted to form water, is able to readsorb even where the surface coverage of CO remains high. At the low relative partial pressures of water used, however, there was no effect of added water on the formation of methane. The surface residence time of water determined from isotopic transients contains the residence time on the surface during the primary formation reaction as well as the time spent during readsorption(s). Part II addressed how a catalyst modifier (in this case Cl) affects methanation in CO hydrogenation using steady-state isotopic transient kinetic analysis (SSITKA) of methanation. The results obtained using silica-supported Ru suggest the structural rearrangements induced by the presence of chlorine, rather than selective site blocking or electronic interactions, may be the primary mechanism of chlorine modification of the catalytic properties of supported metals for CO hydrogenation. SSITKA indicated that the decrease in methanation activity with increasing initial Cl concentration was a function of a decrease in the number of reactive surface intermediates (or sites) and not of a change in site activity. 36 refs., 10 figs., 5 tabs.

• Research Organization: Pittsburgh Univ., PA (USA). Dept. of Chemical and Petroleum Engineering
• DOE Contract Number: FG02-86ER13624
• OSTI ID: 6566396
• Report Number(s): DOE/ER/13624-T1; ON: TI89005033
• Country of Publication: United States
• Language: English

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CARBON COMPOUNDS
CARBON MONOXIDE
CARBON OXIDES
CATALYST SUPPORTS
CATALYTIC EFFECTS
CHALCOGENIDES
CHEMICAL REACTIONS
CHLORINE
DOCUMENT TYPES
ELEMENTS
HALOGENS
HYDROGEN COMPOUNDS
HYDROGENATION
METALS
METHANATION
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MOLECULAR STRUCTURE
NICKEL
NONMETALS
OXIDE MINERALS
OXIDES
OXYGEN COMPOUNDS
PLATINUM METALS
POWDERS
PROGRESS REPORT
RUTHENIUM
SILICA
SILICON COMPOUNDS
SILICON OXIDES
SPECIFICITY
SURFACE PROPERTIES
TRANSITION ELEMENTS
WATER