Carbon and carbon monoxide hydrogenation on nickel: support effects

Journal Article · Sat Oct 01 00:00:00 EDT 1983 · J. Catal.; (United States)

DOI:https://doi.org/10.1016/0021-9517(83)90053-2· OSTI ID:5715359

Ozdogan, S Z; Gochis, P D; Falconer, J L

Hydrogenation of carbon, deposited on nickel catalysts by CO disproportionation, was investigated by temperature-programmed surface reaction (TPSR) for four oxide supports, alumina (Al/sub 2/O/sub 3/), silica (SiO/sub 2/), titanium oxide (TiO/sub 2/), and SiO/sub 2/.Al/sub 2/O/sub 3/. The rate of carbon monoxide hydrogenation was measured by temperature-programmed reaction (TPR) for comparison. The rate of carbon hydrogenation to methane was found to be independent of the support and an average activation energy of 42 kJ/mol was estimated. In contrast, the rate of carbon monoxide hydrogenation was very sensitive to the catalyst support. Nickel (Ni) supported on TiO/sub 2/ exhibited the highest specific activity, and two distinct sites for methanation were observed on Ni/TiO/sub 2/ and Ni/Al/sub 2/O/sub 3/. The lowest specific activities were observed for Ni/SiO/sub 2/ and Ni/SiO/sub 2/.Al/sub 2/O/sub 3/. For all catalysts, carbon hydrogenation occurred at a lower temperature than carbon monoxide hydrogenation. For both TPR and TPSR, small amounts of ethane were formed and at a lower temperature than methane. The amount of less-active, ..beta..-carbon observed in TPSR experiments was very small on all catalysts. These results indicate that at high coverages, carbon hydrogenation does not depend on the support, and thus it is not rate-determining for CO hydrogenation in excess hydrogen. The support is also shown to change the specific rate of carbon monoxide methanation; activity differences seen in steady-state experiments are not just due to differences in site densities. 5 figures, 5 tables.

• Research Organization: Univ. of Colorado, Boulder
• OSTI ID: 5715359
• Journal Information: J. Catal.; (United States), Journal Name: J. Catal.; (United States) Vol. 83:2; ISSN JCTLA
• Country of Publication: United States
• Language: English

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ACTIVATION ENERGY
ADSORPTION
ALKANES
ALUMINIUM COMPOUNDS
ALUMINIUM OXIDES
CARBON
CARBON COMPOUNDS
CARBON MONOXIDE
CARBON OXIDES
CATALYST SUPPORTS
CATALYSTS
CATALYTIC EFFECTS
CHALCOGENIDES
CHEMICAL REACTION KINETICS
CHEMICAL REACTIONS
COMPARATIVE EVALUATIONS
DATA
DISPERSIONS
ELEMENTS
ENERGY
ETHANE
EXPERIMENTAL DATA
HIGH TEMPERATURE
HYDROCARBONS
HYDROGEN
HYDROGENATION
INFORMATION
KINETICS
MEDIUM TEMPERATURE
METALS
METHANATION
METHANE
MINERALS
MIXTURES
NICKEL
NONMETALS
NUMERICAL DATA
ORGANIC COMPOUNDS
OXIDE MINERALS
OXIDES
OXYGEN COMPOUNDS
PROGRAMMING
PULSE TECHNIQUES
REACTION KINETICS
SAMPLE PREPARATION
SILICA
SILICON COMPOUNDS
SILICON OXIDES
SORPTION
SORPTIVE PROPERTIES
SURFACE PROPERTIES
SYNTHESIS
TEMPERATURE DEPENDENCE
TEMPERATURE MEASUREMENT
TIME DEPENDENCE
TITANIUM COMPOUNDS
TITANIUM OXIDES
TRANSITION ELEMENT COMPOUNDS
TRANSITION ELEMENTS