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Title: Hydrodesulfurization catalysis by Chevrel-phase compounds

Thesis/Dissertation ·
OSTI ID:6365801

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/. X-ray powder diffraction and laser Raman spectroscopy analysis of the used catalysts revealed that the bulk structures were stable under reaction conditions. Using a deuterium-thiophene feed at 400/sup 0/C, the amount of deuterium incorporated into thiophene and into the desulfurization products (hydrogen sulfide, butadiene, and butenes) 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; only small amounts of HDS and D/sub 2/S were detected. At the same levels of thiophene conversion, unpromoted MoS/sub 2/ introduced up to 10 times more deuterium into the nondesulfurized thiophene than 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.

Research Organization:
Iowa State Univ. of Science and Technology, Ames (USA)
DOE Contract Number:
W-7405-ENG-82
OSTI ID:
6365801
Resource Relation:
Other Information: Thesis (Ph. D.)
Country of Publication:
United States
Language:
English