Reduced molybdenum oxidation states in hydrodesulfurization catalysis by Chevrel phases
The catalytic activities of reduced (relative to Mo{sup 4+}) molybdenum sulfides, known as Chevrel phases, have been evaluated for thiophene and benzothiophene hydrosulfurization (HDS) and 1-butene hydrogenation (HYD). These materials have been found to have HDS activities comparable to, or greater than, model unpromoted and cobalt-promoted MoS{sub 2} catalysts; in contrast, Chevrel phases exhibit low activities for 1-butene HYD. X-ray powder diffraction and laser Raman spectroscopy analysis of the used (10 hours of thiophene reaction) catalysts indicated that the bulk structures were stable under reaction conditions. XPS analysis demonstrated that reduced molybdenum oxidation states were present at the surface, compared to the Mo{sup 4+} state of the MoS{sub 2} catalysts. The effect of the oxidation state of molybdenum on the catalytic HDS of thiophene was investigated using a series of lead-lutetium Chevrel phases with compositions of Lu{sub 1.2x}PbMo{sub 6}S{sub 8} for 0 {le} x {le} 0.2, and Lu{sub 1.2x}Pb{sub 1{minus}x}Mo{sub 6}S{sub 8} for 0.2 < x {le}1. These same materials were used to evaluate the chemisorption of O{sub 2} and NO as probe molecules of catalytically active sites. 179 refs., 20 figs., 8 tabs.
- Research Organization:
- Ames Lab., IA (United States)
- Sponsoring Organization:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- DOE Contract Number:
- W-7405-ENG-82
- OSTI ID:
- 5339706
- Report Number(s):
- IS-T-1412; ON: DE91018168
- Country of Publication:
- United States
- Language:
- English
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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
400201* -- Chemical & Physicochemical Properties
ALLOYS
CATALYTIC EFFECTS
CHALCOGENIDES
CHEMICAL REACTIONS
CHEMISORPTION
COHERENT SCATTERING
DESULFURIZATION
DIFFRACTION
ELECTRON SPECTROSCOPY
ELEMENTS
HETEROCYCLIC COMPOUNDS
LASERS
LEAD ADDITIONS
LEAD ALLOYS
LUTETIUM ADDITIONS
LUTETIUM ALLOYS
MOLYBDENUM COMPOUNDS
MOLYBDENUM SULFIDES
NITRIC OXIDE
NITROGEN COMPOUNDS
NITROGEN OXIDES
NONMETALS
ORGANIC COMPOUNDS
ORGANIC SULFUR COMPOUNDS
OXIDES
OXYGEN
OXYGEN COMPOUNDS
PHOTOELECTRON SPECTROSCOPY
POLYCYCLIC SULFUR HETEROCYCLES
POWDERS
RAMAN SPECTRA
RARE EARTH ADDITIONS
RARE EARTH ALLOYS
REDUCTION
REFRACTORY METAL COMPOUNDS
SCATTERING
SEPARATION PROCESSES
SORPTION
SPECTRA
SPECTROSCOPY
SULFIDES
SULFUR COMPOUNDS
THIOPHENE
TRANSITION ELEMENT COMPOUNDS
X-RAY DIFFRACTION