EP0173107B1 - Verfahren zur Herstellung von Reformerfeed und Heizöl oder Diesel aus Kohle - Google Patents

Verfahren zur Herstellung von Reformerfeed und Heizöl oder Diesel aus Kohle Download PDF

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Publication number
EP0173107B1
EP0173107B1 EP85109669A EP85109669A EP0173107B1 EP 0173107 B1 EP0173107 B1 EP 0173107B1 EP 85109669 A EP85109669 A EP 85109669A EP 85109669 A EP85109669 A EP 85109669A EP 0173107 B1 EP0173107 B1 EP 0173107B1
Authority
EP
European Patent Office
Prior art keywords
gas
phase hydrogenation
liquid
oil
phase
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
EP85109669A
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German (de)
English (en)
French (fr)
Other versions
EP0173107A1 (de
Inventor
Werner Dr. Döhler
Ludwig Dr. Merz
Heinz Frohnert
Bernd Uckermann
Ulrich Dr. Graeser
Alfons Dr. Jankowski
Eckard Dr. Wolowski
Hans-Friedrich Tamm
Norbert Wilczok
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Veba Oel Technologie und Automatisierung GmbH
Original Assignee
Veba Oel Technologie und Automatisierung GmbH
Priority date (The priority date 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 date listed.)
Filing date
Publication date
Priority claimed from DE3428783A external-priority patent/DE3428783C2/de
Application filed by Veba Oel Technologie und Automatisierung GmbH filed Critical Veba Oel Technologie und Automatisierung GmbH
Publication of EP0173107A1 publication Critical patent/EP0173107A1/de
Application granted granted Critical
Publication of EP0173107B1 publication Critical patent/EP0173107B1/de
Expired legal-status Critical Current

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Classifications

    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10G—CRACKING 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
    • C10G1/00—Production of liquid hydrocarbon mixtures from oil-shale, oil-sand, or non-melting solid carbonaceous or similar materials, e.g. wood, coal
    • C10G1/002—Production of liquid hydrocarbon mixtures from oil-shale, oil-sand, or non-melting solid carbonaceous or similar materials, e.g. wood, coal in combination with oil conversion- or refining processes
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F02—COMBUSTION ENGINES; HOT-GAS OR COMBUSTION-PRODUCT ENGINE PLANTS
    • F02B—INTERNAL-COMBUSTION PISTON ENGINES; COMBUSTION ENGINES IN GENERAL
    • F02B3/00—Engines characterised by air compression and subsequent fuel addition
    • F02B3/06—Engines characterised by air compression and subsequent fuel addition with compression ignition

Definitions

  • the invention relates to a method for producing reformer feed and heating oil or diesel from coal in a bottom phase hydrogenation and a subsequent catalytic gas phase hydrogenation of the type specified in the preamble of claim 1.
  • DE-PS 900 214 describes how, in a process for removing foreign gases from the cycle gas, the high-pressure catalytic hydrogenation of coal, pitch, tars, oils, coal extracts or similar products, consisting of a sump and gas phase system, without the aid of a special washer system ,
  • the liquid reaction product of the gas phase chambers is used directly in the gas phase chamber system as a washing liquid for the gas circuit of the sump phase chamber systems contaminated by gaseous hydrocarbons, nitrogen and carbon monoxide, the sump and gas phase circuits being connected on the pressure and suction sides via a circulation pump system and all the hydrogen in the common cycle is given.
  • all of the hydrogen is fed to the gas phase chambers and the difference between the total gas requirement of the gas phase chambers and the hydrogen added is taken from the pressure side of the common circuit and thus washed from the impurities in the gas phase.
  • the object of the invention is to enable a lowering of the operating pressures required in gas phase hydrogenation to approximately 50-200 bar and to significantly reduce the hydrogen consumption compared to the known method which works in the gas phase hydrogenation at hydrogen partial pressures of over 300 bar.
  • the hydrogenation gas processed in the gas phase hydrogenation represents a hydrogenation gas which is suitable for the bottom phase hydrogenation in quantitative and qualitative terms and which is largely free in particular of the impurities carbon monoxide, carbon dioxide, but also hydrogen sulfide and ammonia.
  • the amount of hydrogen made available by this is sufficient to cover the theoretically necessary hydrogen consumption in the bottom phase hydrogenation.
  • the inventive method is further developed in that the total pressure in the gas phase hydrogenation is designed to be lower than the pressure in the bottom phase hydrogenation.
  • Another object of the invention is to design the circuit of the gas circuits in a method according to the preamble of claim 1 in such a way that the temperature in the gas phase reactor can be regulated.
  • this further object is achieved in that the total fresh hydrogen stream is divided into a subset which is fed to the gas phase feed before entering the gas phase hydrogenation and the remaining subset which is conducted as quench gas for temperature control in the gas phase hydrogenation (claim 3).
  • the pressure in the gas phase is at least about 50 bar lower than the pressure used in the bottom phase or the bottom phase is operated at a pressure of 100 to 400 bar and the gas phase at a pressure of 50 to 200 bar .
  • the integrated coal oil refining provided by the method according to the invention is characterized in particular by a special switching of the gas circuits for the gas phase and the sump phase, in that a cycle gas system is only provided in the sump phase or additionally in the gas phase, but separately from the sump phase and fresh hydrogen only the gas phase hydrogenation is supplied, moreover by a substantial reduction in the pressure required in the gas phase hydrogenation compared to the known method.
  • 2500 m3 of hydrogen are required to produce and process 1 t of coal oil.
  • a quantity ratio of hydrogen to oil of 2500 m 3 / t of coal oil in the gas phase and a chemical hydrogen consumption of, for example, 500 m 3 / t of coal oil 2000 m 3 of hydrogen can be released from the impurities carbon monoxide and carbon dioxide, but also hydrogen sulfide, ammonia and the like is largely free to be released for the bottom phase hydrogenation, so that this provides an amount of hydrogen that is still above the theoretically necessary hydrogen consumption of the bottom phase hydrogenation.
  • the pure high-pressure hydrogen used in the process according to the invention which at coupled processing of the coal oil contained interfering components H 2 0, NH 3 , H 2 S, CO, C0 2 and which also does not contain the hydrogen partial pressure reducing C1 to C 4 gases, causes the catalyst in gas phase hydrogenation to work much more selectively.
  • the pressure reduction made possible according to the invention in the stage of gas phase hydrogenation in comparison to the process of further processing of the coal oil according to the prior art has favorable effects on the technical effort required and thus on the investment cost requirement.
  • the reduced pressure also leads to less through-hydrogenation of the coal oil.
  • the absence of the interfering components CO and C0 2 results in reduced hydrogen consumption, since these would be hydrogenated to hydrocarbons.
  • the light oil obtained by the process according to the invention has reached the reformer feed quality and, after reforming, has excellent motor properties such as. B. a high research octane number and a high engine octane number.
  • the medium oil has met the quality of a heating oil or diesel fuel.
  • the quantitative ratio of hydrogen to coal oil when adding the fresh hydrogen used in the gas phase hydrogenation is 1000 to 5000, preferably 1500 to 3000 m 3 / t coal oil (claim 8).
  • the outflow of the gas phase hydrogenation is cooled according to claim 9 in an energy-efficient manner by heat exchange with the oncoming gas phase hydrogenation subjected to coal oil, with a corresponding heating of the coal oil to be used taking place.
  • the operating temperature can also be kept constant by partially dissipating the heat of hydrogenation and regulating the heating of the fresh hydrogen and the coal oil.
  • a further advantageous embodiment of the method according to the invention is to cool the effluent from the bottom phase hydrogenation after removal of the residue-containing fraction by heat exchange with the mash used, and to further cool it after separating off the fraction serving as mashing oil, the discharge of a waste water containing ammonia and hydrogen sulfide in particular is carried out and the cycle gas, which contains mainly carbon monoxide, carbon dioxide and volatile hydrocarbons and mainly hydrogen, is subjected to an oil wash at about 50 ° C. to room temperature under system pressure or after relaxation.
  • the liquid fraction obtained as coal oil can be further expanded before being fed into the gas phase hydrogenation and separated from the resulting gaseous constituents, after which they may be brought back to the pressure required for the gas phase hydrogenation becomes.
  • the cycle gas of the bottom phase is preheated according to claim 12 in an energy-efficient manner together with the mash by heat exchange with the effluent obtained after removal of the residue-containing fraction from the bottom phase hydrogenation.
  • 0.50 t of the coal oil produced in the process are passed via line 1 after heating by heat exchange in heat exchanger 2 with 1250 m 3 of fresh hydrogen via a top heater 4 and via line 5 via the gas phase catalyst fixedly arranged in the gas phase reactor 6.
  • the gas phase catalyst is a commercially available refining contact based on Ni-Mo aluminum oxide.
  • the cycle gas is fed to the bottom phase hydrogenation via a corresponding compression stage, compressor 15.
  • the mash produced from ground coal with a fraction branched off from the effluent from the bottom phase hydrogenation is further heated and compressed in a furnace 19 after compression by means of a high-pressure pump 16 and after combination with the compressed recycle gas via line 17 and heat exchanger 18 in the heat exchange with the residue-free effluent from the bottom phase hydrogenation fed to the bottom phase hydrogenation in reactor 20.
  • the product leaving the bottom phase reactor 20 then passes through a hot separator 21, from which a stream containing solids is discharged via line 22, which is worked up further.
  • the supplied mash from an intermediate separator 23 removes the fraction serving as mashing oil, line 24, from the solid-free products leaving the head in the hot separator 21.
  • a cooler 25 is further cooled to about 50 ° C to room temperature and in a separating device 26 into a waste water, line 27, a gaseous stream, line 28, which flows through a gas scrubber 29 with discharge of an exhaust gas, line 30, to the recycle gas 14, is given and produced coal oil separated, which after partial relaxation over a Throttle valve and line 1, as indicated above, the gas phase hydrogenation is supplied.

Landscapes

  • 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)
EP85109669A 1984-08-04 1985-08-01 Verfahren zur Herstellung von Reformerfeed und Heizöl oder Diesel aus Kohle Expired EP0173107B1 (de)

Applications Claiming Priority (4)

Application Number Priority Date Filing Date Title
DE3428783 1984-08-04
DE3428783A DE3428783C2 (de) 1984-08-04 1984-08-04 Verfahren zur Herstellung von Reformerfeed und Heizöl oder Diesel aus Kohle
DE3516084 1985-05-04
DE3516084 1985-05-04

Publications (2)

Publication Number Publication Date
EP0173107A1 EP0173107A1 (de) 1986-03-05
EP0173107B1 true EP0173107B1 (de) 1989-02-01

Family

ID=25823581

Family Applications (1)

Application Number Title Priority Date Filing Date
EP85109669A Expired EP0173107B1 (de) 1984-08-04 1985-08-01 Verfahren zur Herstellung von Reformerfeed und Heizöl oder Diesel aus Kohle

Country Status (9)

Country Link
US (1) US4639310A (pl)
EP (1) EP0173107B1 (pl)
CN (1) CN1003375B (pl)
AU (1) AU576714B2 (pl)
BR (1) BR8503655A (pl)
CA (1) CA1238287A (pl)
DE (1) DE3568056D1 (pl)
PL (1) PL145304B1 (pl)
SU (1) SU1563596A3 (pl)

Families Citing this family (6)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US4569749A (en) * 1984-08-20 1986-02-11 Gulf Research & Development Company Coal liquefaction process
US4795841A (en) * 1987-04-02 1989-01-03 Elliott Douglas C Process for upgrading biomass pyrolyzates
DE3741105A1 (de) * 1987-12-04 1989-06-15 Veba Oel Entwicklungs Gmbh Verfahren zur hydrierung fluessiger kohlenstoffhaltiger einsatzstoffe
US20090232725A1 (en) * 2007-11-23 2009-09-17 Sherman Aaron Flow rate of gas in fluidized bed during conversion of carbon based material to natural gas and activated carbon
US9688934B2 (en) * 2007-11-23 2017-06-27 Bixby Energy Systems, Inc. Process for and processor of natural gas and activated carbon together with blower
WO2009067266A1 (en) * 2007-11-23 2009-05-28 Robert Walker Apparatus and method for converting carbonacious material containing hydrogen deficient carbon into diesel fuel

Family Cites Families (20)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US3652446A (en) * 1969-11-17 1972-03-28 Exxon Research Engineering Co Combination process for liquefaction of coal and catalytic cracking of selected fractions thereof
US3755137A (en) * 1971-03-24 1973-08-28 Hydrocarbon Research Inc Multi-stage ebullated bed coal-oil hydrogenation and hydrocracking process
US3892654A (en) * 1974-03-04 1975-07-01 Us Interior Dual temperature coal solvation process
US4048054A (en) * 1976-07-23 1977-09-13 Exxon Research And Engineering Company Liquefaction of coal
US4045328A (en) * 1976-07-23 1977-08-30 Exxon Research And Engineering Company Production of hydrogenated coal liquids
US4189371A (en) * 1976-08-20 1980-02-19 Exxon Research & Engineering Co. Multiple-stage hydrogen-donor coal liquefaction process
US4111788A (en) * 1976-09-23 1978-09-05 Hydrocarbon Research, Inc. Staged hydrogenation of low rank coal
US4123347A (en) * 1976-12-22 1978-10-31 Exxon Research & Engineering Co. Coal liquefaction process
US4330391A (en) * 1976-12-27 1982-05-18 Chevron Research Company Coal liquefaction process
US4330389A (en) * 1976-12-27 1982-05-18 Chevron Research Company Coal liquefaction process
US4222844A (en) * 1978-05-08 1980-09-16 Exxon Research & Engineering Co. Use of once-through treat gas to remove the heat of reaction in solvent hydrogenation processes
US4159236A (en) * 1978-05-12 1979-06-26 Gulf Oil Corporation Method for combining coal liquefaction and gasification processes
US4338182A (en) * 1978-10-13 1982-07-06 Exxon Research & Engineering Co. Multiple-stage hydrogen-donor coal liquefaction
US4452688A (en) * 1979-09-04 1984-06-05 Electric Power Research Institute Integrated coal liquefication process
US4300996A (en) * 1979-12-26 1981-11-17 Chevron Research Company Three-stage coal liquefaction process
US4410414A (en) * 1980-01-18 1983-10-18 Hybrid Energy Systems, Inc. Method for hydroconversion of solid carbonaceous materials
US4322283A (en) * 1980-09-04 1982-03-30 Exxon Research & Engineering Co. Coal conversion in the presence of added hydrogen sulfide
US4485008A (en) * 1980-12-05 1984-11-27 Exxon Research And Engineering Co. Liquefaction process
US4400263A (en) * 1981-02-09 1983-08-23 Hri, Inc. H-Coal process and plant design
DE3105030A1 (de) * 1981-02-12 1982-09-02 Basf Ag, 6700 Ludwigshafen Verfahren zur kontinuierlichen herstellung von kohlenwasserstoffoelen aus kohle durch druckhydrierung in zwei stufen

Also Published As

Publication number Publication date
AU4515485A (en) 1986-02-06
EP0173107A1 (de) 1986-03-05
DE3568056D1 (en) 1989-03-16
CN85108007A (zh) 1986-10-29
CA1238287A (en) 1988-06-21
PL145304B1 (en) 1988-08-31
CN1003375B (zh) 1989-02-22
SU1563596A3 (ru) 1990-05-07
PL254799A1 (en) 1986-06-17
US4639310A (en) 1987-01-27
AU576714B2 (en) 1988-09-01
BR8503655A (pt) 1986-05-06

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