Novel Bimetallic Dispersed Catalysts for Temperature-programmed Coal Liquefaction PDF Download
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Languages : en
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Pages : 247
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Development of new catalysts is a promising approach to more efficient coal liquefaction. It has been recognized that dispersed catalysts are superior to supported catalysts for primary liquefaction of coals, because the control of initial coal dissolution or depolymerization requires intimate contact between the catalyst and coal. This research is a fundamental and exploratory study on catalytic coal liquefaction, with the emphasis on exploring novel bimetallic dispersed catalysts for coal liquefaction and the effectiveness of temperature-programmed liquefaction using dispersed catalysts. The primary objective of this research was to explore novel bimetallic dispersed catalysts from organometallic molecular precursors, that could be used in low concentrations but exhibit relatively high activity for efficient hydroliquefaction of coals under temperature-programmed conditions. We have synthesized and tested various catalyst precursors in liquefaction of subbituminous and bituminous coals and in model compound studies to examine how do the composition and structure of the catalytic precursors affect their effectiveness for coal liquefaction under different reaction conditions, and how do these factors affect their catalytic functions for hydrogenation of polyaromatic hydrocarbons, for cleavage of C-C bonds in polycyclic systems such as 4-(1-naphthylmethyl)bibenzyl, for hydrogenolysis of C-O bond such as that in dinaphthylether, for hydrodeoxygenation of phenolic compounds and other oxygen-containing compounds such as xanthene, and for hydrodesulfurization of polycyclic sulfur compounds such as dibenzothiophene. The novel bimetallic and monometallic precursors synthesized and tested in this project include various Mo- and Fe-based compounds.
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Languages : en
Pages : 17
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Development of new catalysts is a promising approach to more efficient coal liquefaction. It has been recognized that dispersed catalysts can be superior to supported catalysts for primary liquefaction of coals, because the control of initial coal dissolution or depolymerization requires intimate contact between the catalyst and coal. The primary objective of this research is to explore novel bimetallic dispersed catalysts from heterometallic molecular precursors, that can be used in low concentrations but exhibit high activity for efficient hydroliquefaction of coals under temperature-programmed conditions. This quarterly report describes the preparation of two precursors. The first is a heterometallic complex consisting of two transition metals, Mo and Ni, and sulfur in a single molecule synthesized. The second is a thiocubane type cluster consisting of iron and sulfur.
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Pages : 41
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This quarterly report describes recent work on two related subjects: (1) effect of dispersed molybdenum catalyst precursor and the influence of water addition on C-O bond cleavage, aromatic hydrogenation and hydrodeoxygenation under coal liquefaction conditions, and (2) the effect of dispersed molybdenum catalyst precursor on the molecular weight reduction and desulfurization of petroleum resids related to coal/petroleum resids coprocessing. Technical progress on the C-O bond cleavage of 2,2(prime)-dinaphthyl ether and high temperature simulated distillation GC and HDS study on catalytic upgrading of atmospheric and vacuum resids.
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Pages : 33
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Coal liquefaction involves cleavage of methylene, dimethylene and ether bridges connecting polycyclic aromatic units and the reactions of various oxygen functional groups. Here in this quarterly, we report on our continued effort on hydrodeoxygenation of O-containing polycyclic model compounds using novel organometallic catalyst precursors. Compounds containing oxygen functional groups, especially phenols, are undesirable components of coal-derived liquids. Removal of these compounds from the products of coal liquefaction is required. A beneficial alternative would be the removal of these compounds, or the prevention of their formation, during the liquefaction reaction itself, rather than as a separate processing step. A novel organometallic catalyst precursor containing Co and Mo has been studied as a potential hydrogenation catalyst for coal liquefaction. To ascertain the hydrodeoxygenation activity of this catalyst under liquefaction conditions, model compounds were investigated. Anthrone, 2,6-di-t-butyl-4-methyl-phenol, dinaphthyl ether, and xanthene were reacted in the presence of the Co-Mo catalyst precursor and a precursor containing only Mo over a range of temperatures, providing a comparison of conversions to deoxygenated products. These conversions give an indication of the hydrodeoxygenating abilities of organometallic catalyst precursors within a coal liquefaction system. For example, at 400°C dinaphthylether was converted 100% (4.5% O-containing products) in the presence of the Co-Mo organometallic precursor, compared to 76.5% conversion (7.4% O-products) in the presence of the Mo catalyst.
