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US4155832A Expired / Lapsed US ⏱️ 0.0 years remaining

Hydrogenation process for solid carbonaceous materials

Assignee: United States Department of Energy
•
Filing: 1977-12-23
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Granted: 1979-05-22
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Expires: 1997-12-23
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Abstract

Abstract Coal or other solid carbonaceous material is contacted with an organic solvent containing both hydrogen and a transition metal catalyst in solution to hydrogenate unsaturated bonds within the carbonaceous material. This benefaction step permits subsequent pyrolysis or hydrogenolysis of the carbonaceous fuel to form gaseous and liquid hydrocarbon products of increased yield and quality.

Inventors

  • 👤 John L. Cox
  • 👤 Wayne A. Wilcox

Bibliographic Details

Application Number —
Jurisdiction US
Data Source google_patents
Last Synchronized 2026-10-26 10:12
CPC Classifications
C; C10; C10G; C10G1/00; C10G1/08; C10G1/086; C10G1/002; C10G1/083

Claims Analysis

Total Claims: 12
Claim 1
Independent Claim 98 words
A method of hydrogenating solid carbonaceous fuels that contain unsaturated carbon to carbn bonds, the carbonaceous materials are selected from coal, lignite, wood, lignin, oil shale, tar sand, peat, and solid petroleum residuals comprising providing an organic solution containing a nickel Zeigler catalyst prepared from a nickel carboxylate reacted with an alkyl aluminum in an anhydrous, organic solvent to provide a homogeneous catalytic solution; treating the catalytic solution with a source of hydrogen to form a hydrogen-containing complex with the transition metal; and contacting the solid carbonaceous material with the catalytic solution to hydrogenate the unsaturated carbon bonds.
Claim 2
Independent Claim 98 words
A method of hydrogenating solid carbonaceous fuels that contain unsaturated carbon to carbn bonds, the carbonaceous materials are selected from coal, lignite, wood, lignin, oil shale, tar sand, peat, and solid petroleum residuals comprising providing an organic solution containing a nickel Zeigler catalyst prepared from a nickel carboxylate reacted with an alkyl aluminum in an anhydrous, organic solvent to provide a homogeneous catalytic solution; treating the catalytic solution with a source of hydrogen to form a hydrogen-containing complex with the transition metal; and contacting the solid carbonaceous material with the catalytic solution to hydrogenate the unsaturated carbon bonds.
Claim 3
Dependent Claim 23 words
The method of claim 1 wherein the solid carbonaceous fuel is contacted with the catalytic solution at a temperature less than 400° C.
Claim 4
Dependent Claim 15 words
The method of claim 2 wherein the temperature is between 150° C. to 350° C.
Claim 5
Independent Claim 20 words
The method of claim wherein the hydrogenated, solid, carbonaceous material is separated from the catalytic solution by a liquid-solid separation.
Claim 6
Dependent Claim 21 words
The method of claim 1 wherein the organic solution includes a liquid solvent of liquefaction products of the solid carbonaceous material.
Claim 7
Dependent Claim 32 words
The method of claim 1 wherein the solid carbonaceous material following the hydrogenation reaction is heated to a temperature substantially in excess of 300° C. to produce gaseous and liquid hydrocarbon products.
Claim 8
Dependent Claim 59 words
The method of claim 6 wherein the solid, hydrogenated carbonaceous material is heated to a temperature of about B 400°-500° C. at about 100-200 atmospheres pressure in the presence of a transition metal catalyst and a source of hydrogen to provide hydrogenolysis of the carbonaceous material resulting in gaseous hydrocarbons, liquid hydrocarbon and solid char containing residual carbonaceous material.
Claim 9
Dependent Claim 38 words
The method of claim 7 wherein the solid char containing residual carbonaceous material is contacted with steam and oxygen to produce a gas containing hydrogen and carbon monoxide as a source of hydrogen for treating the catalytic solution.
Claim 10
Independent Claim 163 words
A method of converting solid carbonaceous material, that includes unsaturated carbon to carbon bonds, selected from coal, lignite, wood, lignin, oil shale, tar sand, peat and solid petroleum residuals to liquid and gaseous hydrocarbon fuels comprising: contacting said solid carbonaceous material with a liquid catalytic solution in the presence of a source of hydrogen at a first temperature below 350° C. to hydrogenate unsaturated carbon bonds within the solid carbonaceous material, said catalytic solution including an organic solvent and a complex compound selected from the group consisting of the carbonyls, hydrocarbonyls and Ziegler-type catalytic compounds of the group VIII transition metals; separating said liquid catalytic solution from said hydrogenated, solid carbonaceous material, and recycling said catalytic solution with dissolved catalyst into contact with fresh carbonaceous material; heating said hydrogenated, solid carbonaceous material to a second temperature in excess of said first temperature in the presence of a hydrogen containing gas to break carbon to carbon bonds and form liquid and gaseous hydrocarbon fuels.
Claim 11
Independent Claim 163 words
A method of converting solid carbonaceous material, that includes unsaturated carbon to carbon bonds, selected from coal, lignite, wood, lignin, oil shale, tar sand, peat and solid petroleum residuals to liquid and gaseous hydrocarbon fuels comprising: contacting said solid carbonaceous material with a liquid catalytic solution in the presence of a source of hydrogen at a first temperature below 350° C. to hydrogenate unsaturated carbon bonds within the solid carbonaceous material, said catalytic solution including an organic solvent and a complex compound selected from the group consisting of the carbonyls, hydrocarbonyls and Ziegler-type catalytic compounds of the group VIII transition metals; separating said liquid catalytic solution from said hydrogenated, solid carbonaceous material, and recycling said catalytic solution with dissolved catalyst into contact with fresh carbonaceous material; heating said hydrogenated, solid carbonaceous material to a second temperature in excess of said first temperature in the presence of a hydrogen containing gas to break carbon to carbon bonds and form liquid and gaseous hydrocarbon fuels.
Claim 12
Dependent Claim 16 words
The method of claim 9 wherein said first temperature is between 150° C. and 350° C.

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USPTO Annuity & Maintenance Windows

Annuity Stage Window Opens Payment Deadline Surcharge Period Until Estimated Fee Status
3.5 Years (Year 4) 1982-05-21 1982-11-20 1983-05-22 $2000.00 Window Closed / Lapsed
7.5 Years (Year 8) 1986-05-21 1986-11-20 1987-05-22 $3760.00 Window Closed / Lapsed
11.5 Years (Year 12) 1990-05-21 1990-11-20 1991-05-22 $7700.00 Window Closed / Lapsed

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