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Title: Catalytic hydrogenation of solvent-refined lignite to liquid fuels. [5 refs. ; autoclave studies at 375-450/sup 0/C and H/sub 2/ pressure 1500-4500 psi; Ni-Mo-Al/sub 2/O/sub 3/; Co-Mo-Al/sub 2/O/sub 3/; Ni-W-Al/sub 2/O/sub 3/; Ni-W-SiO/sub 2/-Al/sub 2/O/sub 3/; Al/sub 2/O/sub 3/; SnCl/sub 2/; presulfided Ni-Mo-Al/sub 2/O/sub 3/; Co-Mo-Al/sub 2/O/sub 3/; Ni-W-Al/sub 2/O/sub 3/]

Abstract

Solvent-refined lignite (SRL) can be produced by treating lignite (not dried) with CO-H/sub 2/, donor solvent and high temperature. This reactive black solid softens at about 150/sup 0/C, is soluble in many organic solvents, is very low in ash and sulfur, and appears to be a good feedstock for further upgrading. Thus, a wide-ranging study was undertaken to determine the best reducing conditions for converting SRL to light distillable liquid fuels and/or chemical feedstocks. Batch autoclave studies were carried out in the temperature range of 375-450/sup 0/C, hydrogen pressure range of 1500-4500 psi, with catalysts Ni-Mo-Al/sub 2/O/sub 3/, Co-Mo-Al/sub 2/O/sub 3/, Ni-W-Al/sub 2/O/sub 3/. Ni-W-SiO/sub 2/-Al/sub 2/O/sub 3/, SiO/sub 2/-Al/sub 2/O/sub 3/, Al/sub 2/O/sub 3/,SnCl/sub 2/, and presulfided catalysts Ni-Mo-Al/sub 2/O/sub 3/, Co-Mo-Al/sub 2/O/sub 3/, Ni-W-Al/sub 2/O/sub 3/. Varying amounts of the solvents tetrahydrofuran, tetralin, napthalene, and FS-120 petroleum fraction were also studied. Reductions without any solvent were studied too and were quite successful. The results were evaluated in terms of the amount of light liquids produced, deoxygenation, denitrification, hydrogen-carbon ratios, aromatic-aliphatic hydrogen ratios, and benzene solubility of unconverted material. Best results were obtained with a presulfided Ni-Mo-Al/sub 2/O/sub 3/ catalyst at 450/sup 0/C, operating pressure of about 3500 psimore » with a 1:1 SRL-tetralin solvent ratio (90 percent overall conversion, approx.20 percent light liquid (1), 15 percent light oil (2), 20 percent heavy oil (3 and 4), 10 percent unconverted). However, operating without any solvent also gave satisfactory results (88 percent overall conversion, 40 percent light liquid, 10 percent light oil, 10 percent heavy oil, 12 percent unconverted. Detailed gas chromatography-mass spectrometry (GC-MS) studies of selected liquid fractions indicate a high degree of aromaticity as tetralins, hydrophenanthrenes, and hydropyrenes.« less

Authors:
 [1]; ; ; ; ;
  1. Univ. of North Dakota, Grand Forks
Publication Date:
OSTI Identifier:
7344081
Resource Type:
Journal Article
Journal Name:
Energy Sources; (United States)
Additional Journal Information:
Journal Volume: 3:1
Country of Publication:
United States
Language:
English
Subject:
01 COAL, LIGNITE, AND PEAT; LIGNITE; REDUCTION; SOLUBILITY; SOLVENT-REFINED COAL; HYDROGENATION; ALUMINIUM OXIDES; AROMATICS; ASHES; AUTOCLAVES; CARBON MONOXIDE; CATALYSTS; CATALYTIC EFFECTS; COBALT; DENITRIFICATION; EFFICIENCY; GAS CHROMATOGRAPHY; HIGH PRESSURE; HIGH TEMPERATURE; HYDROGEN; MASS SPECTROSCOPY; MOLYBDENUM; NICKEL; ORGANIC SOLVENTS; PRODUCTION; SILICON OXIDES; SOLVENT PROPERTIES; SULFUR; TIN CHLORIDES; TUNGSTEN; ALUMINIUM COMPOUNDS; BROWN COAL; CARBON COMPOUNDS; CARBON OXIDES; CARBONACEOUS MATERIALS; CHALCOGENIDES; CHEMICAL REACTIONS; CHLORIDES; CHLORINE COMPOUNDS; CHROMATOGRAPHY; COAL; CRYOGENIC FLUIDS; ELEMENTS; ENERGY SOURCES; FLUIDS; FOSSIL FUELS; FUELS; HALIDES; HALOGEN COMPOUNDS; METALS; NONMETALS; ORGANIC COMPOUNDS; OXIDES; OXYGEN COMPOUNDS; REFRACTORY METALS; RESIDUES; SEPARATION PROCESSES; SILICON COMPOUNDS; SOLVENTS; SPECTROSCOPY; TIN COMPOUNDS; TIN HALIDES; TRANSITION ELEMENTS; 010403* - Coal & Coal Products- Hydrogenation- (-1987); 010407 - Coal & Coal Products- Solvent Extraction- (-1987)

Citation Formats

Low, J Y.F., Klabunde, K J, Woolsey, N F, Baltisberger, R J, Govek, M, and Stenberg, V I. Catalytic hydrogenation of solvent-refined lignite to liquid fuels. [5 refs. ; autoclave studies at 375-450/sup 0/C and H/sub 2/ pressure 1500-4500 psi; Ni-Mo-Al/sub 2/O/sub 3/; Co-Mo-Al/sub 2/O/sub 3/; Ni-W-Al/sub 2/O/sub 3/; Ni-W-SiO/sub 2/-Al/sub 2/O/sub 3/; Al/sub 2/O/sub 3/; SnCl/sub 2/; presulfided Ni-Mo-Al/sub 2/O/sub 3/; Co-Mo-Al/sub 2/O/sub 3/; Ni-W-Al/sub 2/O/sub 3/]. United States: N. p., 1976. Web. doi:10.1080/00908317608945965.
Low, J Y.F., Klabunde, K J, Woolsey, N F, Baltisberger, R J, Govek, M, & Stenberg, V I. Catalytic hydrogenation of solvent-refined lignite to liquid fuels. [5 refs. ; autoclave studies at 375-450/sup 0/C and H/sub 2/ pressure 1500-4500 psi; Ni-Mo-Al/sub 2/O/sub 3/; Co-Mo-Al/sub 2/O/sub 3/; Ni-W-Al/sub 2/O/sub 3/; Ni-W-SiO/sub 2/-Al/sub 2/O/sub 3/; Al/sub 2/O/sub 3/; SnCl/sub 2/; presulfided Ni-Mo-Al/sub 2/O/sub 3/; Co-Mo-Al/sub 2/O/sub 3/; Ni-W-Al/sub 2/O/sub 3/]. United States. https://doi.org/10.1080/00908317608945965
Low, J Y.F., Klabunde, K J, Woolsey, N F, Baltisberger, R J, Govek, M, and Stenberg, V I. 1976. "Catalytic hydrogenation of solvent-refined lignite to liquid fuels. [5 refs. ; autoclave studies at 375-450/sup 0/C and H/sub 2/ pressure 1500-4500 psi; Ni-Mo-Al/sub 2/O/sub 3/; Co-Mo-Al/sub 2/O/sub 3/; Ni-W-Al/sub 2/O/sub 3/; Ni-W-SiO/sub 2/-Al/sub 2/O/sub 3/; Al/sub 2/O/sub 3/; SnCl/sub 2/; presulfided Ni-Mo-Al/sub 2/O/sub 3/; Co-Mo-Al/sub 2/O/sub 3/; Ni-W-Al/sub 2/O/sub 3/]". United States. https://doi.org/10.1080/00908317608945965.
@article{osti_7344081,
title = {Catalytic hydrogenation of solvent-refined lignite to liquid fuels. [5 refs. ; autoclave studies at 375-450/sup 0/C and H/sub 2/ pressure 1500-4500 psi; Ni-Mo-Al/sub 2/O/sub 3/; Co-Mo-Al/sub 2/O/sub 3/; Ni-W-Al/sub 2/O/sub 3/; Ni-W-SiO/sub 2/-Al/sub 2/O/sub 3/; Al/sub 2/O/sub 3/; SnCl/sub 2/; presulfided Ni-Mo-Al/sub 2/O/sub 3/; Co-Mo-Al/sub 2/O/sub 3/; Ni-W-Al/sub 2/O/sub 3/]},
author = {Low, J Y.F. and Klabunde, K J and Woolsey, N F and Baltisberger, R J and Govek, M and Stenberg, V I},
abstractNote = {Solvent-refined lignite (SRL) can be produced by treating lignite (not dried) with CO-H/sub 2/, donor solvent and high temperature. This reactive black solid softens at about 150/sup 0/C, is soluble in many organic solvents, is very low in ash and sulfur, and appears to be a good feedstock for further upgrading. Thus, a wide-ranging study was undertaken to determine the best reducing conditions for converting SRL to light distillable liquid fuels and/or chemical feedstocks. Batch autoclave studies were carried out in the temperature range of 375-450/sup 0/C, hydrogen pressure range of 1500-4500 psi, with catalysts Ni-Mo-Al/sub 2/O/sub 3/, Co-Mo-Al/sub 2/O/sub 3/, Ni-W-Al/sub 2/O/sub 3/. Ni-W-SiO/sub 2/-Al/sub 2/O/sub 3/, SiO/sub 2/-Al/sub 2/O/sub 3/, Al/sub 2/O/sub 3/,SnCl/sub 2/, and presulfided catalysts Ni-Mo-Al/sub 2/O/sub 3/, Co-Mo-Al/sub 2/O/sub 3/, Ni-W-Al/sub 2/O/sub 3/. Varying amounts of the solvents tetrahydrofuran, tetralin, napthalene, and FS-120 petroleum fraction were also studied. Reductions without any solvent were studied too and were quite successful. The results were evaluated in terms of the amount of light liquids produced, deoxygenation, denitrification, hydrogen-carbon ratios, aromatic-aliphatic hydrogen ratios, and benzene solubility of unconverted material. Best results were obtained with a presulfided Ni-Mo-Al/sub 2/O/sub 3/ catalyst at 450/sup 0/C, operating pressure of about 3500 psi with a 1:1 SRL-tetralin solvent ratio (90 percent overall conversion, approx.20 percent light liquid (1), 15 percent light oil (2), 20 percent heavy oil (3 and 4), 10 percent unconverted). However, operating without any solvent also gave satisfactory results (88 percent overall conversion, 40 percent light liquid, 10 percent light oil, 10 percent heavy oil, 12 percent unconverted. Detailed gas chromatography-mass spectrometry (GC-MS) studies of selected liquid fractions indicate a high degree of aromaticity as tetralins, hydrophenanthrenes, and hydropyrenes.},
doi = {10.1080/00908317608945965},
url = {https://www.osti.gov/biblio/7344081}, journal = {Energy Sources; (United States)},
number = ,
volume = 3:1,
place = {United States},
year = {Thu Jan 01 00:00:00 EST 1976},
month = {Thu Jan 01 00:00:00 EST 1976}
}