Mechanism of formation oxygenated compounds from CO + H[sub 2] reaction over SiO[sub 2]-supported Ru-Co bimetallic carbonyl cluster-derived catalysts

Journal Article · Sun Nov 01 04:00:00 EST 1992 · Journal of Catalysis; (United States)

DOI:https://doi.org/10.1016/0021-9517(92)90018-D· OSTI ID:5518303

Xiao, Feng-Shou ^[1]; Fukuoka, A; Ichikawa, M ^[2]

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1. Hokkaido Univ., Sapporo (Japan) Jilin Univ., Changchun (China)
2. Hokkaido Univ., Sapporo (Japan)

The catalytic performance in CO hydrogenation over Ru, Ru-Co, and Co carbonyl cluster-derived catalysts has been investigated, and it was found that the activity and selectivity for oxygenated products on a series of Ru-Co/SiO[sub 2] catalysts are much higher than those on Ru[sub 3]/SiO[sub 2] and Co[sub 4]/SiO[sub 2] catalysts. The mechanism of oxygenated formation on these Ru-Co/SiO[sub 2] catalysts has been investigated by in situ infrared, mass, and X-ray photoelectron spectroscopies. The IR spectra of reaction of CO + H[sub 2] with Ru-Co/SiO[sub 2] catalysts show a band appearing at 1584 cm[sup [minus]1], which has a good relationship to the activity and selectivity for oxygenates in CO hydrogenation. The adsorption of CO on reduced Ru-Co/SiO[sub 2] catalysts prepared from Ru-Co bimetallic carbonyl clusters exhibits a band at 1680 cm[sup [minus]1] shifting to 1640 cm[sup [minus]1] with [sup 13]CO, which is assigned to the C- and O-ended CO chemisorbed on Ru-Co/SiO[sub 2] catalysts. The chemical trapping of 1584 cm[sup [minus]1] adspecies shows that the 1584 cm[sup [minus]1] species reacts with H[sub 2] to produce CH[sub 4] and CH[sub 3]OH, and the addition of D[sub 2] to 1584 cm[sup [minus]1] species results in the formation of CHD[sub 3] and CHD[sub 2]OD. With the increase of reaction time and temperature, the author finds the bands at 1555 and 1440-1470 cm[sup [minus]1], while the 1584 cm[sup [minus]1] band gradually decreases on Ru-Co/SiO[sub 2] catalysts. XPS spectra demonstrate that the Ru and Co sites on the surface of Ru-Co/SiO[sub 2] catalysts are in the chemical state of Ru[sup 0] and Co[sup 2[minus]], respectively, and it is suggested that the bimetallic Ru[sup 0]-Co[sup 2+] sites are very active centers for the formation of oxygenates in CO hydrogenation. 62 refs., 19 figs., 5 tabs.

• OSTI ID: 5518303
• Journal Information: Journal of Catalysis; (United States), Journal Name: Journal of Catalysis; (United States) Vol. 138:1; ISSN 0021-9517; ISSN JCTLA5
• Country of Publication: United States
• Language: English

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