On the Preferred Active Sites of Promoted MoS2 for Hydrodesulfurization with Minimal Organonitrogen Inhibition
详细信息 查看全文
- 作者：Srinivas Rangarajan ; Manos Mavrikakis
- 刊名：ACS Catalysis
- 出版年：2017
- 出版时间：January 6, 2017
- 年：2017
- 卷：7
- 期：1
- 页码：501-509
- 全文大小：594K
- ISSN：2155-5435
文摘
Hydrodesulfurization is a process to produce ultralow-sulfur diesel fuel. Although promoted molybdenum sulfide (MoS2) catalysts have been used industrially for several decades, the active site requirements for selective hydrodesulfurization of organosulfur compounds with minimal inhibition by organonitrogen constituents of a real gasoil feed has not been resolved. Using molecular binding energy descriptors derived from plane wave density functional theory calculations for comparative adsorption of organosulfur and organonitrogen compounds, we analyzed more than 20 potential sites on unpromoted and Ni- and Co-promoted MoS2. We find that hydrogen sulfide and ammonia are simple descriptors of adsorption of sterically unhindered organosulfur and organonitrogen compounds such as dibenzothiophene and acridine, respectively. Further, organonitrogen compounds in gasoil bind more strongly than organosulfur compounds on all sites except on sites with exposed metal atoms on the corner and sulfur edges of promoted MoS2. Consequently, these sites are proposed as required for maximum-hydrodesulfurization minimum-inhibition catalysis.