Hydrogenation of organic oxygenates on Ni/Al[sub 2]O[sub 3] and Ni/SiO[sub 2] catalysts

Journal Article · Sun May 01 00:00:00 EDT 1994 · Journal of Catalysis; (United States)

DOI:https://doi.org/10.1006/jcat.1994.1115· OSTI ID:7288153

Chen, B; Falconer, J L ^[1]

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1. Univ. of Colorado, Boulder, CO (United States)

Temperature-programmed reaction (TPR) was used to compare the hydrogenation rates of adsorbed methanol, ethanol, 1-propanol, dimethyl ether, formic acid, acetaldehyde, acetone, and methoxy (formed from coadsorbed CO and H[sub 2]) on a Ni/Al[sub 2]O[sub 3] catalyst. The oxygenates adsorb on the Al[sub 2]O[sub 3] support, and hydrogenation involves a spillover process since H[sub 2] dissociates on the Ni surface. The rates of hydrogenation to CH[sub 4] are essentially the same for all the oxygenates studied. Apparently, the same rate-determining step, reverse spillover of an oxygenated species from Al[sub 2]O[sub 3] to Ni, limits the formation of CH[sub 4]. Similar processes occur on Ni/SiO[sub 2] for methanol and ethanol, but their coverages on SiO[sub 2] are a factor of 15 lower and hydrogenation to CH[sub 4] takes place over a broad temperature range. None of the oxygenates remained on the Ni surface of Ni/Al[sub 2]O[sub 3] in H[sub 2] flow; apparently they spilled over to the Al[sub 2]O[sub 3] or were hydrogenated at room temperature. On Ni/SiO[sub 2], only HCOOH adsorbs and dissociates on Ni to form adsorbed CO. Coadsorption shows that [sup 13]CO and various oxygenates have independent adsorption and hydrogenation behavior. 56 refs., 10 figs., 2 tabs.

• OSTI ID: 7288153
• Journal Information: Journal of Catalysis; (United States), Journal Name: Journal of Catalysis; (United States) Vol. 147:1; ISSN 0021-9517; ISSN JCTLA5
• Country of Publication: United States
• Language: English

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ACETALDEHYDE
ACETONE
ALCOHOLS
ALDEHYDES
ALUMINIUM COMPOUNDS
ALUMINIUM OXIDES
CARBOXYLIC ACIDS
CATALYSIS
CATALYST SUPPORTS
CATALYTIC EFFECTS
CHALCOGENIDES
CHEMICAL REACTIONS
ELEMENTS
ETHERS
FORMIC ACID
HETEROGENEOUS CATALYSIS
HYDROGENATION
HYDROXY COMPOUNDS
KETONES
METALS
MONOCARBOXYLIC ACIDS
NICKEL
ORGANIC ACIDS
ORGANIC COMPOUNDS
ORGANIC OXYGEN COMPOUNDS
OXIDES
OXYGEN COMPOUNDS
SILICON COMPOUNDS
SILICON OXIDES
TRANSITION ELEMENTS