United States Patent: 4152248

 

We believe some extended preamble to be needed in this report.

First, though not documented herein, available literature confirms that both named inventors in the United States Patent we enclose, via the above link, were employed at the USDOE's Argonne National Laboratory, just south of Chicago, Illinois.

And, in this US Patent, with ownership of the rights assigned to the United States Government, is confirmed a fact that we have, from other sources, already documented:

Primary and carbonaceous Coal liquids can be hydrogenated, to form hydrocarbon petroleum substitute materials, through catalyzed reactions with a hydrogen-rich synthesis gas itself derived from Coal.

Our Government much prefers to use non-identifying and more generic terms and phrases like "gas mixture including hydrogen"; but, from deep within the bowels of the full Disclosure, we submit this one, and only one, excerpted passage which explains where we would get such a "gas mixture"; as follows:

"The hydrogen and carbon monoxide gas stream can be obtained conveniently from the product of a coal gasification process."

Our USDOE is more clear about the origination of the Coal liquids to be so treated, with that conveniently obtained "hydrogen and carbon monoxide gas stream", in their process; as they specify in several places, for example, that:

"The coal liquids produced by well-known coal liquefaction processes include a mixture of aromatic compounds including but not limited to benzene, naphthalene, anthracene, methylindan, decalin and derivatives of these compounds (and, the) term 'coal liquid' is intended to include carbonaceous liquids derived from anthracite, bituminous, and lignite coal as well as ... related materials."

And:

"It is desirable to further hydrogenate these coal liquids and separate them from solid materials to make them suitable for use as fuel oils and feed stock for the production of refined fuels."

Further, we assert that the entire technology, as herein disclosed by our USDOE, is, in fact, merely an adaptation of, and variation on, long-known petroleum refinery operations - conventional oil refining processes labeled commonly in the petroleum industry as "hydro-treating" and "hydro-refining".

Those are techniques that have, for many decades, been routinely applied to "heavy" crudes and petroleum refinery "bottoms", to upgrade them into the same sorts of "feed stock for the production of refined fuels".

The USDOE also specifies, in this Coal hydrogenation and liquefaction process, the need for, and use of, a "dissociating solvent", for the primary Coal liquids such as naphthalene and anthracene; and, the DOE identifies appropriate examples of such solvent as being "ethylene glycol, propylene glycol (and) glycerol".

It might interest you to know that, as confirmed by multiple web-based references, the first United States commercial-scale ethylene glycol production facility was fired up in 1925, in South Charleston, WV, by one of the companies that later became Union Carbide Corporation.

And, the ethylene glycol was made there out of Coal.

All of that said, our following, more extended, excerpts should fill in a few more details of how our own United States government figured out, more than three decades ago, ways to react what are, in essence, Coke oven tars, blended into a solvent which can be made from Coal, with, again in essence, Coke oven gasses mixed with Steam, to synthesize hydrocarbon liquids suitable for use as "fuel oils" and as "feed stock for the production of refined fuels":

"United States Patent 4,152,248 - Hydrogenation of Coal Liquid

Date: May, 1979

Inventors: Harold Feder and Jerome Rathke, Illinois

Assignee: The United States of America

Abstract: Coal liquid having a dissolved transition metal catalyst ... is hydrogenated with hydrogen gas or a hydrogen donor. A dissociating solvent contacts the coal liquid during hydrogenation to form an immiscible liquid mixture at a high carbon monoxide pressure. The dissociating solvent, e.g. ethylene glycol, is of moderate coordinating ability, while sufficiently polar to solvate the transition metal as a complex cation along with a transition metal, carbonyl anion in solution at a decreased carbon monoxide pressure. The carbon monoxide pressure is reduced and the liquids are separated to recover the hydrogenated coal liquid as product. The dissociating solvent with the catalyst in ionized form is recycled to the hydrogenation step at the elevated carbon monoxide pressure for reforming the catalyst complex within fresh coal liquid.

The invention described herein was made in the course of, or under, a contract with the United States Department of Energy.

Claims: A method of hydrogenating a coal liquid through use of a transition metal, carbonyl catalyst dissolved as a complex molecule in said coal liquid comprising: mixing the coal liquid including said dissolved catalyst with a dissociating solvent selected from the group of hydroxylic liquids consisting of ethylene glycol, propylene glycol, glycerol ... and mixtures thereof, in the presence of a gas mixture including hydrogen to hydrogenate the coal liquid, said gas mixture including carbon monoxide ... .

(And) separating the hydrogenated coal liquid as product from the dissociating solvent ...; and recycling the dissociating solvent ... to mix with fresh coal liquid.

(And) wherein said dissociating solvent includes ethylene glycol (and/or) an ethylene glycol-water mixture containing up to 20% by weight water.

The catalyst is dicobalt octacarbonyl as a complex molecule dissolved in the coal liquid and a solvated cobaltous cation along with tetracarbonyl cobaltate anion dissolved within the glycol. Also, the inventors have found that this combination of glycol and catalyst preferentially sweeps mineral matter including ash and other solid particles from the coal liquid into the glycol phase to permit their separation from the product.

The coal liquids produced by well-known coal liquefaction processes include a mixture of aromatic compounds including but not limited to benzene, naphthalene, anthracene, methylindan, decalin and derivatives of these compounds. Tars, bitumens, asphaltenes, other higher boiling compounds and ash may also be included. It is desirable to further hydrogenate these coal liquids and separate them from solid materials to make them suitable for use as fuel oils and feed stock for the production of refined fuels.

In addition, high-molecular-weight coal tars, bitumens, asphaltenes, coal particles and ash may be in the coal liquid feed. 

The hydrogen and carbon monoxide gas stream can be obtained conveniently from the product of a coal gasification process. Consequently, other gases such as methane, nitrogen, oxygen and carbon dioxide may be included."

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So, not only can we hydrogenate primary Coal tars, even if they still contain ash, after they've been dissolved in a liquid we can make from Coal, using a gas mixture we can make from Coal, to synthesize  "feed stock for the production of refined fuels", but:

We, as a nation, learned, as herein officially, how to do just that - in fact, paid through our taxes to learn how to do just that - more than three decades ago.

When will we, as a nation, learn, publicly, that we can convert our abundant Coal so efficiently into such "feed stock for the production of refined fuels"?


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