CA1155411A - Process for hydrogenation of coal - Google Patents

Process for hydrogenation of coal

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Publication number
CA1155411A
CA1155411A CA000359665A CA359665A CA1155411A CA 1155411 A CA1155411 A CA 1155411A CA 000359665 A CA000359665 A CA 000359665A CA 359665 A CA359665 A CA 359665A CA 1155411 A CA1155411 A CA 1155411A
Authority
CA
Canada
Prior art keywords
coal
hydrogenation
gases
slurry
coal slurry
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Expired
Application number
CA000359665A
Other languages
French (fr)
Inventor
Helmut Wurfel
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Individual
Original Assignee
Individual
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Filing date
Publication date
Application filed by Individual filed Critical Individual
Application granted granted Critical
Publication of CA1155411A publication Critical patent/CA1155411A/en
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Classifications

    • CCHEMISTRY; METALLURGY
    • C10PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10GCRACKING HYDROCARBON OILS; PRODUCTION OF LIQUID HYDROCARBON MIXTURES, e.g. BY DESTRUCTIVE HYDROGENATION, OLIGOMERISATION, POLYMERISATION; RECOVERY OF HYDROCARBON OILS FROM OIL-SHALE, OIL-SAND, OR GASES; REFINING MIXTURES MAINLY CONSISTING OF HYDROCARBONS; REFORMING OF NAPHTHA; MINERAL WAXES
    • C10G1/00Production of liquid hydrocarbon mixtures from oil-shale, oil-sand, or non-melting solid carbonaceous or similar materials, e.g. wood, coal
    • C10G1/08Production of liquid hydrocarbon mixtures from oil-shale, oil-sand, or non-melting solid carbonaceous or similar materials, e.g. wood, coal with moving catalysts
    • C10G1/083Production of liquid hydrocarbon mixtures from oil-shale, oil-sand, or non-melting solid carbonaceous or similar materials, e.g. wood, coal with moving catalysts in the presence of a solvent

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  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Oil, Petroleum & Natural Gas (AREA)
  • Life Sciences & Earth Sciences (AREA)
  • Wood Science & Technology (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • General Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Production Of Liquid Hydrocarbon Mixture For Refining Petroleum (AREA)

Abstract

ABSTRACT OF THE DISCLOSURE
In a process for the hydrogenation of coal the coal is mixed with emulsifier oil to form a slurry. In further processing, the coal slurry is pumped to reaction pressure, heated, and subjected to catalytically accelerated hydrogenation in the presence of hydrogen. In subsequent processing at least a portion of the hot products gases occurring in the hydrogenation is thoroughly mixed with the coal slurry, and the remaining product consisting of solids and liquids is hydrogenated.

Description

1~5411 PROCESS FOR HYDROGENATION OF COAL

The invention relates to a process for hydrogenation of coal, in which the coal is mixed with an emulsifier oil to form a slurry.
The slurry is pumped to reaction pressure, heated and is then subjected to catalytically accelerated hydrogenation in the pres-ence of hydrogen.
A process for the hydrogenation of coal is known in which the coal is dried and in pulverized form is mixed with emulsifier oil, and the coal slurry obtained is then pumped to reaction pressure, and is heat exchanged with a portion-of the subsequent reaction products. The slurry is then heated in a preliminary heater to a temperature closa to that of the reaction by bringing in outside heat, and is subsequently hydrogenated in a reactor, in the presence of hydrogen and a suitable catalyst. The product frac-tion leaving the reactor is fractionated in a subsequent heat exchanger into a vaporous main fraction comprising gases, benzenes, and distillation oils, and a liquid base fraction comprising un-rea~ted coal, ashes, catalyst particles, as well as other high-molecular substances which are difficult to hydrogenize, such asasphaltenes, in particular, as well as bitumen and heavy oil.
While the main fraction is cooled by heat exchange with the coal slurry and is being drawn off by the charge, the heavy oil is separated from the base fraction and is utilized as an emulsifier ~5 oil for the incoming coal.
Disadvantages of this known process are its high energy consumption as well as its considerable equipment expense.
Thus the entire coal charge must be dried in a special drier using outside heat. For example, if the charge consists of bitum-inous coal with an average water content of about 8~, the dryingo~ a ton of coal requires an energy output of about 0.1 Gcal Igram calories). Moreover, the coal has to be pulverized in an expensive process to a particle size of <0.1 mm.
In the known process hydrogenation occurs at relatively high pressure, which is due to the fact that in the process of preheat-ing the coal slurry to the hydrogenation start-up temperature of approximately 410C. gas, separating as physically and chemically bound water and lower hydrocarbons ~methane, ethane, etc.) reaches the reactor. This causes a lowering of .~
\ ~ ~

1 1~54~ 1 the partial pressure of the hydrocarbon which only can be compen-sated for by increased total pressure in the reactor resulting in turn in a requirement for increased pump energy and increased equipment expense for reinforcing the reactor and other pressure equipment.
A disadvantage of the known process is that heat exchange for heating the coal slurry has proven to be difficult. As the coal slurry has high viscosity, a uniform introduction of the coal slurry into the areas of the heat exchanger is hard to achieve, and additionally, the further heating of the coal slurry in the preheater presents difficulties since the coal suspended in the slurry greatly expands as a result of the prevailing high tempera-tures. This results in a further increase in viscosity so that in the end, only a pulsating passage of the coal slurry through the preheater is possible, which causes considerable abrasion and wear to the equipment. In this connection, pressure shocks of up to 10 bar can occur.
The objective of the present invention is directed to a pro-cess for the hydrogenation of coal mentioned above, wherein there are improved economics in energy consumption and equipment expense.
The invention achieves this objective in that at least a portion of the hot product gases, resulting from the hydrogenation, are intimately mixed with the coal slurry under pressure, and that the gases can be separated from the resultant mixture of gases, liquids and solids, and the remaining mixture, consisting of solids and liquids, can be hydrogenated.
The intimate mixing of the incoming coal slurry, already pumped to pressure, with the hot gases occurring as a reaction pro-duct at the top of the hydrogenation reactor, or at the top of the heat separator - if there is one subsequent to the reactor -greatl~ enhances heating of the coal slurry Thereby all of the physically bound, and a portion of the chemically bound water contained in the coal is withdrawn. In the course of this heat exchange, the coal is completely dried, and a significant feature is that the usual costly drying step in the coal preparation process, can be dispensed with.
Another important advantage is that due to the high tempera-ture attained by the coal in direct heat exchange with the hot product gases from the hydrogenation, other gases contained in the ~ .

.

1~55411 ~ 3 coal, like methane, ethane and others, are released. The coal entering the hydrogenation process following heat exchange thus is already essentially free of gas, reducing formation of gases in the hydrogenation reactor itself. This in turn leads to an increased hydrogen partial pressure in the reactor, enhancing hydrogenation effectiveness. In comparison to known processes, hydrogenation can now be carried out at a lower total pressure, thereby making it more economical in both initial investment and operating costs.
The combination of gases, liquids and solids, which result from the intimate mixing of the hot product gases and the coal slurry, is fractionated in a heat separator downstream to the mixing device. The heated base product from the separator, now comprising distillation oils condensed from product gases in addition to the coal slurry, is directly carried to the hydrogena-tion reactor. The gases formed at the top of the s~parator are further cooled by the hydrogenation of hydrocarbon. The distilla-tion oils, condensed during cooling, are processed in a distilla-tion facility, while the remaining gases are washed and the hydrocarbon recovered in the process is recycled. Further treat-ment of the recovered distillation oils can be carried out in a distillation facility without difficulty because all non-distilla-ble components, like entrained asphaltenes, and others, which originally were part of the hot product gases in the hydrogenation reactor, have already been washed out in the process of the direct heat exchange with the coal slurry, and together with the slurry, are returned to the hydrogenation reactor.
Another essential advantage of this process is that the heat-ing of the incoming coal slurry to hydrogenation start-up tempera-ture does not require heat exchangers charged with the coal slurry.The largest portion of the heat required is introduced in the form of exothermic reaction heat in the process of mixing the hot product gases. In a further feature of the invention, additional heat which may-be required can be obtained either by heating of the hydrogenation hydrocarbon and/or by mixing the coal slurry - ~ith a heated distillation fraction from the distillation plantr mentioned above.
Moreover, the costly pulverizing of the coal to an average size of ~ 0.1 mm becomes unnecessary as the coal, on its way to ~!

1 P5~41 1 the hydrogenation reactor, only passes through pipes, instead of passing through heat exchangers, where it could cause deposits.
A device for carrying out the process is characterized in that the exit of the high-pressure pump for the incoming coal slurry and the top of the hydrogenation reactor are in communication with the inlet of a mixing device, the exit of the mixing device is in comm-unication with a se~arator, and the bottom of the separator is in communication with the inlet of the hydrogenation reactor. Further details of the invention are depicted by way of a schematic.
The drawing shows schematically a process for the hydrogenatlon of coal, in which the coal to be processed, without previous drying and having a water content of about 6% and a particle size of up to
2 mm, is fed to an emulsifier vessel 4 via line l and is mixed with emulsifier oil which is entering via line 2. The catalysts required for the hydrogenation, e.g. alloys of metals of Groups IV, VI and -~III of the Periodic System, or combinations thereof, are supplied via line 3 and mixed with the coal or sprayed onto it, respectively.
In the emulsifier vessel 4, the slurry has a ratio of 70~ by weight coal to approximately 30% by weight oil.
The coal slurry is pumped to a pressure o~ approximately 200 bar by pump 5 and is carried directly to the lower region of mixing device 8. At the same time, mixing device 8 is supplied with hot product gases from the top of hydrogenation reactor 22 via line 7. These gases, which in addition to hydrogen, water vapor and low-boiling hydrocarbons like methane! ethane, etc.
essentially contain distillation oils in the naphtha-, medium-and heavy oil range, have a temperature of approximately 470C.
and are intimately mixed with the incoming coal slurry in mixing device 8. Mixing device 8 advantageously consists of a simple, vertical pipe.
Due to the rapid mixing, the temperature at the exit of mixing device 8 is approximately 400C., which aids in the removal of all water contained in the coal, and even a portion of the shemically bound water, as well as highly volatile gases, like methane, ethane, etc.
The contents of mixing device 8, having been thoroughly mixed, is directed to separator 9, where it is separated into a gaseous and a solids-liquid phase. The solids-liquid phase, now consisting of dried coal and partially degassed coal, in ~! -.

1~5411 addition to emulsifier oil, heavy oil and entrained asphaltenes from the product gases, which have been condensed and washed out during the mixing process, are now fed directly to hydrogenation reactor 22 by pump 19 via line 20.
The gaseous phase of separator 9 is further cooled and there-by partially condensed in heat exchanger 10, and directed to separator 11. The top product of separator 11 reaches a wash facility 12 and is subjected there to an oil wash. Hydrogen-free residual gas is withdrawn via line 13, while the remaining hydro-gen is mixed with fresh hydrogen entering via line 14, is then carried to heat exchanger 10 via line 17, then to furnace 18 for further heating and finally is returned to the hydrogenation reactor via line 21.
The bottom product of separator 11, essentially a fraction consisting of naptha-, medium-, and heavy oil, as well as water, is directed via line 15 to distillation plant 16, where it is separated into the different product fractions.
If additional heat is required for heating of the fresh coal slurry, a heavy oil fraction is extracted from distillation plant 16, heated in a heat exchanger 26 by an outside heat supply and is then added to the incoming coal slurry, vi-a line 6.
The liquid portion of the product occurring in the hydrogena-tion reactor is directed to vacuum distillation facility 24 via line 23. The heavy oil thus recovered flows in the form of emulsifying oil towards container 4 via line 2, while the solids-containing distillation residue is with drawn from the facility via line 25. The residue can be further processed in a gasifica-tion plant (not depicted) for the production of hydrogen.

. .

Claims (5)

The embodiments of the invention in which an exclusive property or privilege is claimed are defined as follows:-
1. A process for the hydrogenation of coal in which the coal is mixed with emulsifier oil to form a slurry, the coal slurry is pumped to reaction pressure, heated, and subjected to catalytically accelerated hydrogenation in the presence of hydrogen, wherein at least a portion of the hot product gases occurring in the hydrogenation is thoroughly mixed with the coal slurry, pumped to pressure, the gases are separated from the resultant mixture consisting of gases, liquids and solids, and the remaining product consisting of solids and liquids is hydrogenated.
2. A process according to claim 1, wherein the separated gases are further cooled in heat exchange with hydro-genation hydrocarbon.
3. A process according to claim 1 or 2, wherein the hydrogen required for the hydrogenation is heated by an outside heat supply before introduction into the hydrogenation reactor.
4. A process according to claim 1 or 2, wherein the hydrocarbons condensed during cooling of the gases are separated, processed, and at least a portion of the heavy oil recovered in the process is heated and added to the incoming coal slurry, already pumped to pressure.
5. A device for carrying out the process according to claim 1 wherein the outlet of a high-pressure pump for incoming coal slurry and the top of a hydrogen reactor are in communication with the inlet portion of a mixing device, and the outlet of the mixing device is connected to a separator, and the bottom of the separator is in communication with the inlet of the hydrogenation reactor.
CA000359665A 1979-09-06 1980-09-05 Process for hydrogenation of coal Expired CA1155411A (en)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
DEP2936008.5 1979-09-06
DE19792936008 DE2936008A1 (en) 1979-09-06 1979-09-06 METHOD FOR HYDROGENATING COAL

Publications (1)

Publication Number Publication Date
CA1155411A true CA1155411A (en) 1983-10-18

Family

ID=6080194

Family Applications (1)

Application Number Title Priority Date Filing Date
CA000359665A Expired CA1155411A (en) 1979-09-06 1980-09-05 Process for hydrogenation of coal

Country Status (7)

Country Link
JP (1) JPS5655486A (en)
AU (1) AU6209180A (en)
CA (1) CA1155411A (en)
DE (1) DE2936008A1 (en)
GB (1) GB2058125B (en)
PL (1) PL226602A1 (en)
ZA (1) ZA805523B (en)

Families Citing this family (7)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE2943494C2 (en) * 1979-10-27 1987-04-16 Basf Ag, 6700 Ludwigshafen Process for producing liquid hydrocarbons from coal
DE3042984C2 (en) * 1980-11-14 1986-06-26 Saarbergwerke AG, 6600 Saarbrücken Process for hydrogenating coal
DE3141380C2 (en) * 1981-10-17 1987-04-23 GfK Gesellschaft für Kohleverflüssigung mbH, 6600 Saarbrücken Process for hydrogenating coal
DE3246609A1 (en) * 1982-12-16 1984-06-20 GfK Gesellschaft für Kohleverflüssigung mbH, 6600 Saarbrücken METHOD FOR HYDROGENATING COAL
DE3438330C2 (en) * 1983-11-05 1987-04-30 GfK Gesellschaft für Kohleverflüssigung mbH, 6600 Saarbrücken Process for liquefying coal
DE3741105A1 (en) * 1987-12-04 1989-06-15 Veba Oel Entwicklungs Gmbh METHOD FOR HYDROGENATING LIQUID CARBONATED SUBSTANCES
DE3741104A1 (en) * 1987-12-04 1989-06-15 Ruhrkohle Ag METHOD FOR HYDROGENATING SOLID CARBON-CONTAINING SUBSTANCES

Also Published As

Publication number Publication date
DE2936008A1 (en) 1981-04-02
JPS5655486A (en) 1981-05-16
ZA805523B (en) 1981-12-30
GB2058125A (en) 1981-04-08
GB2058125B (en) 1983-03-23
PL226602A1 (en) 1981-05-22
JPS5714792B2 (en) 1982-03-26
AU6209180A (en) 1981-03-19

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