Carbon monoxide and carbon dioxide hydrogenation catalyzed by supported ruthenium carbonyl clusters. A novel procedure for encapsulating Ru/sub 3/(CO)/sub 12/ within the pores of Na-Y zeolite

Journal Article · Wed Aug 24 04:00:00 EDT 1988 · Inorg. Chem.; (United States)

DOI:https://doi.org/10.1021/ic00290a025· OSTI ID:6001412

Hastings, W R; Cameron, C J; Thomas, M J; Baird, M C

Zeolite-supported ruthenium catalysts for the hydrogenation of carbon monoxide and carbon dioxide have been prepared by sorbing Ru(CO)/sub 5/ (molecular diameter 6.3 /angstrom/) onto Na-Y zeolite and Linde 5A molecular sieve. Although the metal carbonyl is not absorbed into the pores of the molecular sieve, it is readily absorbed into the pores and supercages of the Na-Y zeolite. Slow, temperature-programmed heating of the Ru/sub 3/(CO)/sub 12/ in Na-Y to 350/degree/C under a flow of hydrogen results in decarbonylation and formation of a CO hydrogenation catalyst that produces a very atypical (for ruthenium) hydrocarbon distribution truncated at about C/sub 10/. The unusual product distribution presumably arises because the catalyst sites are situated within the zeolite supercages. Thus the metal is highly dispersed and/or the growing hydrocarbon chains are subject to geometrical limitations on their growth. Consistent with this hypothesis, ruthenium carbonyl clusters immobilized on the external surfaces of Na-Y zeolite, Linde 5A molecular sieve, and /gamma/-alumina all exhibit typical, nonselective hydrocarbon product distributions. The same supported ruthenium carbonyl clusters are also extremely active catalysts for the selective hydrogenation of CO/sub 2/(H/sub 2/:CO/sub 2/ = 4:1) to methane. At a lower H/sub 2/:CO/sub 2/ ratio (1:1), however, Na-Y supported Ru/sub 3/(CO)/sub 12/ catalyzes the hydrogenation of CO/sub 2/ to higher hydrocarbons as well (up to C/sub 16/). It is proposed that CO/sub 2/ is reduced to CO and that hydrogenation of both proceeds by the same mechanism. 21 references, 2 figures, 4 tables.

• Research Organization: Queen's Univ., Kingston, Ontario (Canada)
• OSTI ID: 6001412
• Journal Information: Inorg. Chem.; (United States), Journal Name: Inorg. Chem.; (United States) Vol. 27:17; ISSN INOCA
• Country of Publication: United States
• Language: English

Related Subjects

090121* -- Hydrocarbon Fuels-- Chemical Synthesis-- (1976-1989)
10 SYNTHETIC FUELS
CARBON COMPOUNDS
CARBON DIOXIDE
CARBON MONOXIDE
CARBON OXIDES
CARBONYLS
CATALYSIS
CATALYTIC EFFECTS
CHALCOGENIDES
CHEMICAL PREPARATION
CHEMICAL REACTIONS
COMPLEXES
DATA
EXPERIMENTAL DATA
HYDROCARBONS
HYDROGENATION
INFORMATION
NUMERICAL DATA
ORGANIC COMPOUNDS
OXIDES
OXYGEN COMPOUNDS
RUTHENIUM COMPLEXES
SYNTHESIS
TRANSITION ELEMENT COMPLEXES