Hydrodesulfurization catalysis by Chevrel phase compounds
The catalytic activity of Chevrel phase compounds (M/sub x/Mo/sub 6/S/sub 8/) for thiophene hydrodesulfurization at 400/sup 0/C has been found to be comparable to or greater than that of model industrial catalysts (unpromoted and cobalt-promoted MoS/sub 2/). The most active Chevrel phase catalysts were those containing the ''large'' ternary component cations Ho, Pb, Sn; the ''intermediate'' cation materials (M = Ag and In) were less active; the ''small'' cation materials (M = Cu, Fe, Ni, and Co) were the least active catalysts. The 1-butene hydrogenation activities of the Chevrel phase catalysts at 400/sup 0/C were much lower than MoS/sub 2/, with the exception of Ni/sub 1.6/Mo/sub 6/S/sub 8/. X-ray powder diffraction and laser Raman spectroscopy analysis of the used catalysts revealed that the bulk structures were stable under reaction conditions. XPS analysis of the fresh Chevrel phase catalysts showed reduced molybdenum surface oxidation states compared to the Mo/sup +4/ state of MoS/sub 2/ catalysts. After thiophene reaction, various degrees of oxidation of the surface molybdenum states could be detected for the small and intermediate cation materials, with an accompanying loss of the ternary component from the surface. This was not the case for the large cation materials. Using a deuterium-thiophene feed at 400/sup 0/C, the amount of deuterium incorporated into thiophene and into the desulfurization products was determined as a function of reaction time. For all Chevrel phase and MoS/sub 2/ catalysts examined, H/sub 2/S was almost exclusively formed. At the same levels of thiophene conversion, unpromoted MoS/sub 2/ introduced up to 10 times more deuterium into the nondesulfurized thiophene did the ''promoted'' catalysts. A mechanism of thiophene hydrodesulfurization is proposed: butadiene is the initial reaction product and the hydrogen of hydrogen sulfide originates from the hydrogen-exchange of thiophene. 140 refs., 87 figs., 30 tabs.
- Research Organization:
- Ames Lab., IA (USA)
- DOE Contract Number:
- W-7405-ENG-82
- OSTI ID:
- 5911822
- Report Number(s):
- IS-T-1168; ON: DE85011359
- Resource Relation:
- Other Information: Thesis
- Country of Publication:
- United States
- Language:
- English
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Related Subjects
ORGANIC
PHYSICAL AND ANALYTICAL CHEMISTRY
02 PETROLEUM
CATALYSTS
BINDING ENERGY
COMPARATIVE EVALUATIONS
PROMOTERS
RAMAN SPECTRA
STRUCTURAL CHEMICAL ANALYSIS
DESULFURIZATION
CHEMICAL REACTION KINETICS
HYDROGEN SULFIDES
CHEMICAL REACTION YIELD
HYDROGENATION
MOLYBDENUM SULFIDES
CATALYTIC EFFECTS
THIOPHENE
COBALT COMPOUNDS
COPPER COMPOUNDS
DEUTERIUM
DEUTERIUM COMPOUNDS
EXPERIMENTAL DATA
HIGH TEMPERATURE
HOLMIUM COMPOUNDS
INDIUM COMPOUNDS
IRON COMPOUNDS
LEAD COMPOUNDS
MASS SPECTROSCOPY
NICKEL COMPOUNDS
PHOTOELECTRON SPECTROSCOPY
SILVER COMPOUNDS
TIN COMPOUNDS
TRACER TECHNIQUES
X-RAY DIFFRACTION
CHALCOGENIDES
CHEMICAL REACTIONS
COHERENT SCATTERING
DATA
DIFFRACTION
ELECTRON SPECTROSCOPY
ENERGY
HETEROCYCLIC COMPOUNDS
HYDROGEN COMPOUNDS
HYDROGEN ISOTOPES
INFORMATION
ISOTOPE APPLICATIONS
ISOTOPES
KINETICS
LIGHT NUCLEI
MOLYBDENUM COMPOUNDS
NUCLEI
NUMERICAL DATA
ODD-ODD NUCLEI
ORGANIC COMPOUNDS
ORGANIC SULFUR COMPOUNDS
RARE EARTH COMPOUNDS
REACTION KINETICS
REFRACTORY METAL COMPOUNDS
SCATTERING
SPECTRA
SPECTROSCOPY
STABLE ISOTOPES
SULFIDES
SULFUR COMPOUNDS
TRANSITION ELEMENT COMPOUNDS
YIELDS
400301* - Organic Chemistry- Chemical & Physicochemical Properties- (-1987)
400201 - Chemical & Physicochemical Properties
020400 - Petroleum- Processing