MODELING OF SYNGAS REACTIONS AND HYDROGEN GENERATION OVER SULFIDES

Klier, Kamil ; Spirko, Jeffery A. ; Neiman, Michael L.

Lehigh University (United States)

关键词: Hydrocarbons;    Sulfides;    Hydroxides;    08 Hydrogen;    Potassium;   

DOI  :  10.2172/836407
RP-ID  :  NONE
RP-ID  :  FG26-01NT41276
RP-ID  :  836407

美国|英语

来源: UNT Digital Library

【 摘 要 】

The objective of the research is to analyze pathways of reactions of hydrogen with oxides of carbon over sulfides, and to predict which characteristics of the sulfide catalyst (nature of metal, defect structure) give rise to the lowest barriers toward oxygenated hydrocarbon product. Reversal of these pathways entails the generation of hydrogen, which is also proposed for study. During this study, adsorption reactions of H atoms and H{sub 2} molecules with MoS{sub 2}, both in molecular and solid form, have been modeled using high-level density functional theory. The relative stabilities of pure MoS{sub 2} edges were calculated and small clusters exhibiting properties of the edges were modeled. The results were finalized and published in the journal ''Surface Science''. Hydrogen adsorption energies on both the edges and the clusters were calculated, and the thermodynamics of hydrogen adsorption on both systems were evaluated. The adsorption locations and vibrational frequencies were also determined. These additional results were published in a second paper in ''Surface Science''. Most recently, the bonding and effect of alkali and transition metal ions was investigated on the MoS{sub 2} clusters. Potassium atoms bind to the clusters and increase the binding of hydrogen to the clusters while reducing the activation barriers for hydrogen adsorption. Silver attaches to the Mo7S14 cluster and donates its odd electron to the nearby Mo atoms and should have a similar effect to hydrogen as potassium does.