Density Function Theory Study of Hydrodesulfurization Mechanism by Molybdenum Sulfide Clusters

Tanabe, Christopher
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[Honolulu] : [University of Hawaii at Manoa], [August 2016]
In this thesis, we explored the potential energy surfaces of MoSx and Mo3Sx clusters interacting with H2 and methane. We started by looking at the bare MoSx clusters to determine which would most readily combine with other atoms. We narrowed our search down to the MoS3 and MoS4 clusters, then ran geometry optimization calculations on those structures combined with H2 or methane. Once we had a working set of minima structures, we ran calculations to find the transition state structures connecting them. In the 3rd chapter of the thesis we did a similar study on the Mo3Sx clusters. Gold et. al. previously determined that the Mo3Sx clusters with x=6,7,8 are most likely to take part in the hydrodesulfurization reaction. Using the low energy structures from those Mo3Sx clusters as a starting point, we investigated the interactions of methane with the catalyst. We found energetic trends that were consistent with the results of our MoSx calculations. We also found several transition state structures that, along with the corresponding intrinsic reaction coordinate calculations, depicted methanethiol being converted to methane on the Mo3Sx cluster.
M.S. University of Hawaii at Manoa 2016.
Includes bibliographical references.
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