A molecular approach to heterogeneous catalysis. Part 2. 1-Butene isomerization catalyzed by silica-anchored osmium carbonyls
- Northwestern Univ., Evanston, IL (USA)
- CNR, Milano (Italy)
- Universita La Sapienza, Rome (Italy)
The title reaction has been investigated at 115{degree}C using HOs{sub 3}(CO){sub 10}(OSi chemical bond) as catalyst or catalyst precursor. By FTIR and XP spectroscopy and by TPDE, evidence exists for the in situ formation of molecular oxidized osmium moieties, covalently anchored to the surface, which are the active catalytic species. The intermediate formation of an olefin adduct during the in situ decomposition of the cluster precursors is supported by chemical extraction of the surface species and further FTIR and {sup 1}H NMR characterization. The reversible poisoning effect of CO and the beneficial influence of H{sub 2} on the catalytic activity and selectivity are also reported and discussed. The catalytic behavior of preformed oxidized osmium surface species has been found to be markedly dependent on the preparation method. The highest activity was obtained when they are formed in situ in the presence of 1-butene. Silica-supported metallic osmium catalysts displayed different activity and selectivity, thus confirming the molecular nature of the catalytic process.
- OSTI ID:
- 6469473
- Journal Information:
- Journal of Catalysis; (USA), Journal Name: Journal of Catalysis; (USA) Vol. 123:1; ISSN 0021-9517; ISSN JCTLA
- Country of Publication:
- United States
- Language:
- English
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Related Subjects
020400* -- Petroleum-- Processing
ALKENES
BUTENES
CARBON COMPOUNDS
CARBON MONOXIDE
CARBON OXIDES
CARBONYLS
CATALYSIS
CATALYST SUPPORTS
CATALYTIC EFFECTS
CHALCOGENIDES
CHEMICAL PREPARATION
CHEMICAL REACTION KINETICS
CHEMICAL REACTIONS
CONTROL
DECOMPOSITION
ELECTRON SPECTROSCOPY
ELEMENTS
FOURIER TRANSFORMATION
HETEROGENEOUS CATALYSIS
HYDROCARBONS
HYDROGEN
HYDROGEN 1
HYDROGEN ISOTOPES
INFRARED SPECTRA
INTEGRAL TRANSFORMATIONS
ISOMERIZATION
ISOTOPES
KINETICS
LIGHT NUCLEI
MAGNETIC RESONANCE
MEDIUM TEMPERATURE
MOLECULES
NONMETALS
NUCLEAR MAGNETIC RESONANCE
NUCLEI
ODD-EVEN NUCLEI
ORGANIC COMPOUNDS
OSMIUM COMPOUNDS
OSMIUM OXIDES
OXIDES
OXYGEN COMPOUNDS
PHOTOELECTRON SPECTROSCOPY
POISONING
REACTION INTERMEDIATES
REACTION KINETICS
REFRACTORY METAL COMPOUNDS
RESONANCE
SILICON COMPOUNDS
SILICON OXIDES
SPECTRA
SPECTROSCOPY
STABLE ISOTOPES
SURFACE PROPERTIES
SYNTHESIS
TEMPERATURE CONTROL
TRANSFORMATIONS
TRANSITION ELEMENT COMPOUNDS
X-RAY SPECTROSCOPY