Novel catalysts for upgrading coal-derived liquids. Final technical progress report
Research described in this report was aimed at synthesizing and evaluating supported Mo oxynitrides and oxycarbides for the selective removal of nitrogen, sulfur and oxygen from model and authentic coal-derived liquids. The Al{sub 2}O{sub 3}-supported oxynitrides and oxycarbides were synthesized via the temperature programmed reaction of supported molybdenum oxides or hydrogen bronzes with NH{sub 3} or an equimolar mixture of CH{sub 4} and H{sub 2}. Phase constituents and composition were determined by X-ray diffraction, CHN analysis, and neutron activation analysis. Oxygen chemisorption was used to probe the surface structure of the catalysts. The reaction rate data was collected using specially designed micro-batch reactors. The Al{sub 2}O{sub 3}-supported Mo oxynitrides and oxycarbides were competitively active for quinoline hydrodenitrogenation (HDN), benzothiophene hydrodesulfurization (HDS) and benzofuran hydrodeoxygenation (HDO). In fact, the HDN and HDO specific reaction rates for several of the oxynitrides and oxycarbides were higher than those of a commercial Ni-Mo/Al{sub 2}O{sub 3} hydrotreatment catalyst. Furthermore, the product distributions indicated that the oxynitrides and oxycarbides were more hydrogen efficient than the sulfide catalysts. For HDN and HDS the catalytic activity was a strong inverse function of the Mo loading. In contrast, the benzofuran hydrodeoxygenation (HDO) activities did not appear to be affected by the Mo loading but were affected by the heating rate employed during nitridation or carburization. This observation suggested that HDN and HDS occurred on the same active sites while HDO was catalyzed by a different type of site.
- Research Organization:
- Michigan Univ., Ann Arbor, MI (United States). Dept. of Chemical Engineering
- Sponsoring Organization:
- USDOE, Washington, DC (United States)
- DOE Contract Number:
- FG22-92PC92537
- OSTI ID:
- 257335
- Report Number(s):
- DOE/PC/92537--T12; ON: DE96012596
- Country of Publication:
- United States
- Language:
- English
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Related Subjects
ALUMINIUM OXIDES
BENZOFURANS
CATALYST SUPPORTS
CATALYTIC EFFECTS
CHEMICAL COMPOSITION
CHEMICAL PREPARATION
CHEMICAL REACTION KINETICS
COAL LIQUIDS
COMPARATIVE EVALUATIONS
DENITRIFICATION
DESULFURIZATION
EXPERIMENTAL DATA
HYDROGENATION
MOLYBDENUM CARBIDES
MOLYBDENUM NITRIDES
MOLYBDENUM OXIDES
POLYCYCLIC SULFUR HETEROCYCLES
PROGRESS REPORT
QUINOLINES
REDUCTION
REFINING