Catalytic hydrodenitrogenation of quinoline with nanoscale Mo{sub 2}N, Mo{sub 2}C and MoS{sub 2} synthesized by laser pyrolysis
- Univ. of Kentucky, Lexington, KY (United States)
As the quality of available petroleum feedstocks decreases, the demand for better and more active catalysts for hydrotreatment increases. Nitrogen content in coal, tar sands, shale and petroleum residua is present predominantly in the form of heterocyclic compounds. Quinoline constitutes a molecule representative of these heterocyclic compounds and its catalytic denitrogenation is one of the most studied model compound reactions. Nitrogen removal from heterocyclic compounds is a more difficult process than sulfur removal. It has been accepted that it requires hydrogenation of the ring containing the nitrogen atom before hydrogenolysis of the carbon-nitrogen bond occurs. This is partly due to the thermodynamics of the aliphatic C-N bond hydrogenolysis reaction. Figure 1 shows a diagram of the reaction pathway reported by Satterfield et al for the denitrogenation of quinoline over a sulfided NiMo/Al{sub 2}O{sub 3} catalyst. It is seen that the HDN reaction proceeds through the hydrogenation of quinoline (Q) to 1,2,3,4 tetrahydroquinoline (THQ) and 5,6,7,8 tetrahydroquinoline (CBPYD), the first reaction being faster than the second. THQ can either convert into-propylaniline (O-PA), through bond cleavage of the C-N bond, or together with CBPYD, it can hydrogenate to form decahydroquinoline (DHQ). The rapid hydrogenation of Q to THQ causes the establishment of a pseudoequilibrium among this hydrogenated derivatives of quinoline. As seen in the figure, this pathway indicates that removal of nitrogen from O-PA requires the hydrogenation of the aromatic ring, consuming more hydrogen in the reaction. Therefore, it is desirable to synthesize hydrodenitrogenation catalysts that will induce nitrogen removal from the molecule without full hydrogenation of the aromatic ring. This report describes the evaluation of the catalytic activity of molybdenum carbide, molybdenum sulfide, and molybdenum nitride for quinoline hydrodenitrogenation.
- OSTI ID:
- 420495
- Report Number(s):
- CONF-950402-; ISSN 0569-3772; TRN: 97:000006-0031
- Journal Information:
- Preprints of Papers, American Chemical Society, Division of Fuel Chemistry, Vol. 40, Issue 2; Conference: 209. American Chemical Society (ACS) national meeting, Anaheim, CA (United States), 2-6 Apr 1995; Other Information: PBD: 1995
- Country of Publication:
- United States
- Language:
- English
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Related Subjects
36 MATERIALS SCIENCE
NITROGEN
REMOVAL
PETROLEUM
REFINING
MOLYBDENUM NITRIDES
CATALYTIC EFFECTS
MICROSTRUCTURE
MOLYBDENUM CARBIDES
QUINOLINES
CONVERSION
MOLYBDENUM SULFIDES
CATALYSTS
HETEROCYCLIC COMPOUNDS
HYDROGENATION
LIGANDS
REACTION INTERMEDIATES
SURFACE AREA
THERMODYNAMICS
VOLATILITY