Development of unique catalysts for hydrodenitrogenation of coal-derived liquids. Annual report, September 15, 1978-September 14, 1979

Technical Report · Wed Oct 01 00:00:00 EDT 1980

DOI:https://doi.org/10.2172/6835756· OSTI ID:6835756

Katzer, J R; Stiles, A B; Kwart, H

Preliminary results from decahydroquinoline hydrodenitrogenation runs show that Bronsted acidity by itself will not catalyze carbon-nitrogen bond scission. The C-N bond cleavage must therefore be catalyzed by an active site, which consists of a transition metal ion in close proximity to an acid site. It appears that hydrodenitrogenation requires both an acidic and a basic site for the Hoffman E/sub 2/ elimination reaction to occur. Several catalysts have been prepared and tested, including Bronsted and Lewis acid catalysts without metal, and silica-alumina and ..gamma..-alumina impregnated with molybdenum, vanadium, nickel or iron. Our results show that the nitrogen removal rate was highest for molybdenum on ..gamma..-alumina catalyst and the rate decreased with lower Mo concentrations. Aluminum borate and aluminum borate phosphate catalysts (with or without nickel) were prepared to develop novel catalysts that would selectively coordinate the nitrogen atom and remove it without excessive hydrogenation. Results show that the support plays an important role in the nitrogen-removal process. Hydrodenitrogenation of aniline has been studied over a presulfided Ni-Mo/..gamma..-Al/sub 2/O/sub 3/ catalyst, and a reaction network has been proposed. Aniline hydrodenitrogenation appears to involve partial hydrogenation of the benzene ring to reduce aromatic resonance with the nitrogen atom, thus reducing the C-N bond strength and facilitating NH/sub 3/ elimination.

• Research Organization: Delaware Univ., Newark (USA). Dept. of Chemical Engineering
• DOE Contract Number: AS22-78ET03297
• OSTI ID: 6835756
• Report Number(s): DOE/ET/03297-1
• Country of Publication: United States
• Language: English

Related Subjects

01 COAL, LIGNITE, AND PEAT
CATALYSTS
CHEMICAL PREPARATION
PERFORMANCE TESTING
COAL LIQUIDS
DENITRIFICATION
ALUMINIUM COMPOUNDS
BORATES
CATALYTIC EFFECTS
CHEMICAL BONDS
CLEAVAGE
EXPERIMENTAL DATA
HYDROGENATION
MOLYBDENUM
NICKEL
REFINING
STRUCTURAL MODELS
BORON COMPOUNDS
CHEMICAL REACTIONS
CRYSTAL STRUCTURE
DATA
ELEMENTS
FLUIDS
INFORMATION
LIQUIDS
METALS
MICROSTRUCTURE
NUMERICAL DATA
OXYGEN COMPOUNDS
PROCESSING
REFRACTORY METALS
SYNTHESIS
TESTING
TRANSITION ELEMENTS
010405* - Coal
Lignite
& Peat- Hydrogenation & Liquefaction
010402 - Coal
Lignite
& Peat- Purification & Upgrading