EP0556875A2 - Verfahren zur gleichzeitigen Ausscheidung von CO2 und Benzin aus Methan, C2 und höheren Kohlenwasserstoffen und CO2 enthaltenden gasförmigen Kohlenwasserstoffen - Google Patents

Verfahren zur gleichzeitigen Ausscheidung von CO2 und Benzin aus Methan, C2 und höheren Kohlenwasserstoffen und CO2 enthaltenden gasförmigen Kohlenwasserstoffen Download PDF

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Publication number
EP0556875A2
EP0556875A2 EP93107550A EP93107550A EP0556875A2 EP 0556875 A2 EP0556875 A2 EP 0556875A2 EP 93107550 A EP93107550 A EP 93107550A EP 93107550 A EP93107550 A EP 93107550A EP 0556875 A2 EP0556875 A2 EP 0556875A2
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EP
European Patent Office
Prior art keywords
solvent
rich
gas
methane
hydrocarbons
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Granted
Application number
EP93107550A
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English (en)
French (fr)
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EP0556875A3 (en
EP0556875B1 (de
Inventor
Claude Blanc
Henri Paradowski
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Elf Exploration Production SAS
Original Assignee
Societe National Elf Aquitaine
Societe Nationale Elf Aquitaine Production SA
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Publication of EP0556875A3 publication Critical patent/EP0556875A3/fr
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    • 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
    • C10G5/00—Recovery of liquid hydrocarbon mixtures from gases, e.g. natural gas
    • C10G5/04—Recovery of liquid hydrocarbon mixtures from gases, e.g. natural gas with liquid absorbents
    • 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
    • C10G2300/00—Aspects relating to hydrocarbon processing covered by groups C10G1/00 - C10G99/00
    • C10G2300/10—Feedstock materials
    • C10G2300/1025—Natural gas

Definitions

  • the invention relates to a process for the simultaneous decarbonation and degassing of a gaseous mixture consisting mainly of hydrocarbons consisting of methane and hydrocarbons of C 2 and more and also containing C0 2 and optionally one or more non-sulfurized compounds at low point of boiling such as H 2 , CO, N 2 and argon.
  • decarbonation and degassing operations are generally carried out separately and are part of a succession of operations carried out on the gaseous mixture to be treated and mainly comprising an elimination of the acid gas C0 2 , drying, adsorption of the water on a suitable solid such as a molecular sieve, a separation by cryogenic distillation between -30 ° C and -90 ° C associated or not with a solvent extraction in order to obtain the cut of natural gas liquid, and finally reheating the treated gas to ambient temperature in order to generally supply the commercial gas network.
  • the dehydrated and refrigerated natural gas is separated, in a first column (demethanizer) at the head of which is injected an additive consisting of a liquid fraction of C 4 and higher hydrocarbons, in one phase gas containing methane and lighter compounds and a liquid fraction containing C 2 and higher hydrocarbons and C0 2 .
  • This liquid fraction is separated, in a second column (de-ethanizer) into which a certain amount of the additive is also introduced, into an overhead fraction consisting of C0 2 and a bottom fraction containing the C 2 hydrocarbons and more.
  • Said tail fraction is then separated, in a third column, into an overhead fraction consisting of a liquid cut of C 2 to C 4 hydrocarbons and into a tail fraction consisting of a liquid cut of C 4 to C hydrocarbons and plus, which contains most of the butanes and higher hydrocarbons present in the treated natural gas and from which the appropriate quantity is taken to constitute the additive injected in the first and second columns.
  • This additive avoids the crystallization of C0 2 at the top of the demethanizer and ensures the rupture of the azeotrope which forms between ethane and C0 2 and facilitates the separation of these compounds in the deethanizer.
  • the aforementioned process is therefore essentially based on serial distillation operations.
  • the invention provides a process for simultaneous decarbonation and degassing of gas mixtures, which are available under an absolute pressure greater than 0.5 MPa and consist mainly of hydrocarbons consisting of methane and C 2 and more hydrocarbons and also contain C0 2 and optionally one or more low-boiling non-sulfur compounds such as H 2 , CO, N 2 and argon, such gaseous mixtures being for example of the natural gas type, said process making it possible to achieve more easily and at lower cost, in comparison with known processes, the objective of gas mixture in the three components, namely treated gas consisting mainly of methane, liquid cut of hydrocarbons with predominantly C 3 and more hydrocarbons and containing, as required, a more or less significant quantity of ethane and current of C0 2 , which have the specifications defined above.
  • the process according to the invention is of the type of process which is described in the US-A-3770622 quotation and in which the gas mixture is brought into contact, in a washing zone, with a solvent consisting of a liquid which preferentially dissolves C0 2 and C 2 and higher hydrocarbons and which has, on the one hand, at atmospheric pressure, a boiling temperature greater than 40 ° C and, on the other hand, at - 30 ° C, a viscosity less than 0, 1 Pa.s, operating at a sufficiently low temperature and with a ratio of the flow rates of the gaseous mixture to be treated and of the solvent such that, on the one hand, a treated gas consisting mainly of methane and having a molar content is produced in C0 2 at most equal to 2% and, on the other hand, a liquid phase called rich solvent and formed of the solvent enriched in C0 2 and in a fraction of hydrocarbons in C 2 and more containing at least 80 mol% of the hydrocarbons in C 3 and more present in the gauze mixture
  • the process according to the invention differs from the process of the US-A-3770622 citation, and is therefore characterized in that the treatment of the demethanized rich solvent is carried out by subjecting said demethanized rich solvent
  • methane equivalent is meant according to the invention as many pseudo-molecules with a single carbon atom as there are carbon atoms in the considered hydrocarbon molecule.
  • the solvent which is generally defined above for bringing into contact with the gaseous mixture to be treated for the purpose of absorbing C0 2 and C 2 and higher hydrocarbons, preferably has a viscosity of less than 0.05 Pa. s.
  • the solvent according to the invention may consist in particular of one or more liquid absorbents selective for CO 2 and used in anhydrous form or in mixture with water, the said solvent (s) being chosen from the amides of formulas aldehydes of formula formula esters alkanols Ci -C 4 diethers of formula diether alcohols of formula R 9 O- C 2 H 4 - O - C 2 H 4 - OH lactones of formula and propylene carbonate, with in these formulas R 1 and R 2 , identical or different, denoting a hydrogen atom or an alkyl radical in Ci or C 2 , R 3 being an alkyl radical in C 3 or C 4 , R 6 being a C 2 -C 4 alkyl radical or a radical with R 8 denoting an alkyl radical Ci or C 2 and n is 1 or 2, R 7 being an alkyl radical in C 1 -C 2 or a radical Rg denotes an alkyl to C 4 and p is an integer from 2 to 4.
  • Non-limiting examples of liquid organic absorbents corresponding to the above formulas are such as N, N-dimethylformamide, N, N-dimethylacetamide, dimethoxymethane, diethoxymethane, dimethoxy-1,1 ethane, methanol, ethanol, ethylene dimethyl ether glycol, diethylene glycol dimethyl ether, ethylene glycol monomethyl ether, butyrolactone, propiolactone and propylene carbonate.
  • the contacting temperature of the gas mixture to be treated with the solvent in the washing zone is preferably between 0 ° C and -45 ° C.
  • the washing zone advantageously consists of one or more washing columns containing the appropriate number of theoretical washing stages, said columns being, for example, of the type of tray columns or even packed columns.
  • the temperature in each of the washing columns is kept substantially constant by indirect heat exchange, carried out at one or more points of the column in question, between the fluid medium contained in this column and a refrigerating fluid.
  • the demethanization treatment applied to the rich solvent is carried out, in particular, in two stages, namely a first step in which said rich solvent is subjected to a first expansion at an intermediate pressure capable of releasing a large fraction of the methane dissolved in said solvent to demethanize and produce a first gas rich in methane and a premethanized fluid and a second step in which the premethanized fluid is subjected to a second expansion then to a distillation of so as to produce a second methane-rich gas and the demethanized rich solvent, the second methane-rich gas being compressed to the pressure of the first methane-rich gas and then mixed with the latter to form the methane-rich gas phase.
  • the methane-rich gas phase resulting from the demethanization treatment applied to the rich solvent, is advantageously compressed to the pressure of the gas mixture to be treated, then it is cooled and mixed with the gas mixture to be treated before the latter is brought into contact. with the solvent in the washing area.
  • the regeneration of the demethanized rich solvent is carried out by reheating said solvent to a temperature close to ambient, by dividing the reheated solvent into first and second streams, directing the first stream directly to a regeneration zone by directing the second stream to said regeneration zone after having heated it by indirect heat exchange with the regenerated solvent, and by subjecting the solvent to distillation in the regeneration zone.
  • Said distillation can be carried out in the presence of a stream of inert gas, for example nitrogen, injected into the regeneration zone.
  • the gaseous mixture to be treated contains water and / or C 5 and higher hydrocarbons, it is advantageously subjected to a pretreatment intended to remove all or part of these compounds before being brought into contact with the solvent in the washing area.
  • This pretreatment can consist of a distillation possibly carried out in the presence of solvent, taken from the solvent injected into the washing zone, to produce the pretreated gas mixture having a C 6 hydrocarbon content and more than 0.1% by weight, a fraction of so-called heavy hydrocarbons containing almost all of the C 6 and higher hydrocarbons and all or part of the C 5 hydrocarbons and, optionally, a liquid consisting of a mixture of solvent and water.
  • Said distillation of the gas mixture is carried out at a temperature at least equal to the temperature prevailing in the washing zone.
  • the gaseous mixture to be treated arriving via line 1 is introduced into the lower part of a distillation column 2, in which said gaseous mixture is optionally distilled in the presence of solvent withdrawn, through an opening pipe 41 in the upper part of column 2, on the regenerated solvent 38 brought to the washing column 5, before passage of said solvent in a refrigeration zone 39 mounted on the conduit 6 for injecting the regenerated solvent into said washing column 5, so as to produce on the one hand a dried gaseous mixture, evacuated from column 2 by a line 3 and whose hydrocarbon content in C 6 and more is less than 0.1% by weight, and on the other hand a cut hydrocarbon containing almost all of the C 6 and more hydrocarbons and possibly all or part of the C s hydrocarbons, withdrawn from column 2 by a conduit 4 and optionally a liquid withdrawn from the column 2 via a conduit 54 and consisting of a mixture of solvent and water.
  • the dried gaseous mixture leaving column 2 via line 3 is introduced into the lower part of a washing column 5, for example of the plate column type, in which it is brought into contact, countercurrently, with cold solvent regenerated injected into the upper part of column 5 through line 6, after passage through the coolant 39, this contacting being carried out at a temperature of, for example, between 0 ° C and -45 ° C, said temperature being controlled by passage of the liquid medium contained in column 5 in refrigerants 7.
  • a treated gas consisting mainly of methane and depleted in C0 2 is discharged, via a conduit 8, said treated gas being heated in a system 9 for reheating and then directed, via a conduit 10, to a zone of use, while at the bottom of said column 5 is drawn off, via a conduit 11, a liquid phase consisting of the solvent enriched in C0 2 e t other compounds absorbed and called rich solvent.
  • the dried gas mixture is brought into contact with the solvent in the washing column 5 at an appropriate temperature in the range O ° C to -45 ° C and with a ratio of the flow rates of the gas mixture to be treated and of solvent such that on the one hand the treated gas collected, through line 8, at the head of column 5 has a molar content of C0 2 at most equal to 2% and that on the other hand the rich solvent, flowing through the line 11, contains at least 80 mol% of the C 3 and higher hydrocarbons present in the dried gas mixture introduced into column 5.
  • the rich solvent circulating in the conduit 11 is introduced, after passage through the expansion valve 12, into the upper part of an expansion tank 13 in which a first methane-rich gas separates, which is removed at the head of the flask 13 by a conduit 14, and a predemethanized rich solvent, which is withdrawn from the bottom of the flask 13 by a conduit 15.
  • Said predemethanized rich solvent is subjected to a second expansion through an expansion valve 16 followed by a distillation in a distillation column 17 provided with a reboiler 18, so as to produce a second gas rich in methane, which is discharged at the head of column 17 through a pipe 19, and a methane-depleted liquid phase, called demethanized rich solvent, which is drawn off at the bottom of the column 17 through a pipe 27.
  • the second methane-rich gas circulating in the pipe 19 is caused to pass into a compressor 20 from which it exits, via a conduit 21, at a pressure substantially equal to that of the first gas rich in methane passing through the conduit 14, then these two gases rich in methane are mixed in the conduit 22 and the gas phase resulting from this mixture is recycled, by means of a compressor 23, the outlet of which is extended by a conduit 24, a coolant 25 and a conduit 26, in the conduit 3 for supplying the dried gaseous mixture to washing column 5.
  • the regeneration can be carried out in the presence of a stream of inert gas, in particular a stream of nitrogen, injected into the lower part of the column 33 through a conduit 43.
  • Said regeneration produces, on the one hand, a regenerated solvent withdrawn from the bottom of the column 33, through a pipe 34, and used in the heat exchanger 35, to heat the second stream 31 of demethanized rich solvent to be regenerated, before being recycled, by the pump 37 and the conduit 38, towards the washing column 5, and on the other hand a gas mixture discharged at the head of the column 33, by a conduit 42, and containing the C0 2 as well as the C 2 and higher hydrocarbons present in the rich demethanized solvent.
  • the gaseous mixture passing through the conduit 42 is washed against the current, in a washing tower 47 provided with a condenser 46 at the head and a reboiler 70 at the bottom and operating at low temperature, using a hydrocarbon solvent in C 5 and over brought to the washing tower 47 by a conduit 53, said washing producing, on the one hand, a stream 44 of acid gas rich in C0 2 , which contains almost all of the C0 2 present in the solvent rich demethanized and has, expressed in methane equivalent, a hydrocarbon content of less than 10 mol% relative to C0 2 , and, on the other hand, a rich hydrocarbon solvent 45 practically free of C0 2 and containing almost all of the hydrocarbons in C 2 and more present in the gas mixture arriving via line 42.
  • the rich hydrocarbon solvent 45 is brought to a regeneration column 49 in which said solvent 45 is subjected to distillation to produce, on the one hand, a fraction of hydrocarbons 48 constituting the cut of C 2 hydrocarbons and more containing the minus 80 mol% of the C 3 hydrocarbons and more contained in the gas to be treated brought to the washing column 5 by the line 3, and, on the other hand, a regenerated hydrocarbon solvent 50, which is recycled, by the pump 51 , to the washing tower column 47 after refrigeration in the system 52 and passage in the conduit 53.
  • the gaseous mixture to be treated arriving via line 1 with a flow rate of 10,000 kmol / h, a temperature of 30 ° C. and a pressure of 5,000 kPa was introduced into column 2 for elimination of C 6 and higher hydrocarbons. .
  • the gas mixture to be treated being dry, no addition of solvent was carried out via line 41.
  • the pretreated gas mixture was brought into contact with 6000 kmol / h of solvent consisting of a mixture of methanol and water in a molar ratio equal to 95: 5 and having a pressure of 5000 kPa and a temperature equal to -30 ° C. , said contacting being carried out in a washing column 5 comprising 14 plates and operating at - 30 ° C under a pressure of 4900 kPa.
  • the refrigerants 7 fitted to the washing column 5 made it possible to maintain the temperature in said column at the desired value.
  • the heated treated gas is directed through line 10 to an expedition pipeline.
  • the demethanization of the rich solvent firstly involved a first expansion of said solvent at a pressure of 3000 kPa, the expanded relaxed solvent supplying the expansion tank 13 in which 362 kmol / h of a first gas containing 68 mol% of methane were produced. , which was discharged at the head of the flask 13 through line 14, and a predemethanized rich solvent withdrawn from said flask through line 15 and whose molar methane content was reduced from 6.11% to 3.57%.
  • the premethanized rich solvent the temperature of which was equal to -33.6 ° C., was expanded in valve 16 and then fed to the distillation column 17 comprising 10 plates and operating at 1800 kPa.
  • the demethanized rich solvent had the following molar composition:
  • the second methane-rich gas was compressed in compressor 20 to the pressure of the first methane-rich gas, namely 3000 kPa.
  • the compressed gas leaving the compressor 20, via the conduit 21, was mixed with the first methane-rich gas to constitute the methane-rich gas phase 22, which was then compressed, in the compressor 23, until the pressure of the gas mixture a treating, namely 5000 kPa, said compressed gas phase being added through line 24, the refrigerant 25 and line 26, to the pretreated gas mixture circulating in line 3.
  • the compressed methane-rich gaseous phase passing through line 26 had a temperature of -20 ° C, a pressure of 5,000 kPa and a flow rate of 938 kmol / h.
  • the demethanized rich solvent after expansion in the valve 29 and heating in the heating system 28, had a temperature of 10 ° C and a pressure of 800 kpa. Said heated solvent was then divided into a first stream 30 having a flow rate of 4533 kmol / h, which was directed directly to the regeneration column 33, and into a second stream 31, which was heated to 70 ° C. in the heat exchanger. heat 35 before being conveyed to the regeneration column 33.
  • This column operated under a pressure of 700 kPa and included 18 plates, the currents 30 and 31 being injected respectively at the plates 8 and 12, counted from the top of the column.
  • the regeneration column 33 produced at the head a gaseous mixture containing C0 2 and the hydrocarbons in C 2 and more, which was evacuated via line 42 with a temperature of -14 ° C, a pressure of 700 kPa and a flow rate of 2244 kmol / h and at the bottom a regenerated solvent withdrawn from the regeneration column 33 through the pipe 34.
  • the gas mixture passing through line 42 had the following molar composition:
  • the regenerated solvent is cooled by passage through the heat exchanger 35, then recompressed to a pressure of 5000 kPa by the pump 37, and it is then directed through the conduit 38 on the one hand in a major quantity to the washing column 5 , through the refrigerant 39 and the conduit 6.
  • Tower 47 had 35 platforms and operated under a pressure of 700 kPa with a temperature of -30 ° C at the head at the level of the refrigerant 46.
  • the washing tower 47 produced at the head an acid gas stream 44 rich in C0 2 and having a hydrocarbon content, expressed in methane equivalent, of less than 10 mol% with respect to C0 2 , said acid gas stream having a temperature of -30 ° C, a pressure of 650 kPa and a flow rate of 1685 kmol / h, and in the background a hydrocarbon solvent 45 with reduced C0 2 content having a temperature of 95.8 ° C, a pressure of 730 kPa and a flow rate 5059 kmol / h.
  • the molar composition of the acid gas stream 44 was as follows:
  • the rich hydrocarbon solvent 45 had the following molar composition:
  • the fractionation of the rich hydrocarbon solvent 45 in the column 49 provided with 28 trays and operating under a pressure of 600 kPa produced at the head 561 kmol / h of a cut of hydrocarbons 48 in C 2 and more having a temperature of 18 ° C and a pressure of 600 kPa and at the bottom 4500 kmol / h of regenerated hydrocarbon solvent having a temperature of 142.7 ° C and a pressure of 670 kPa, said solvent containing, in mole, 98.89% of hexane and 1, 11% butane.

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  • Chemical & Material Sciences (AREA)
  • Oil, Petroleum & Natural Gas (AREA)
  • Engineering & Computer Science (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • General Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Organic Low-Molecular-Weight Compounds And Preparation Thereof (AREA)
  • Gas Separation By Absorption (AREA)
  • Physical Water Treatments (AREA)
  • Separation Using Semi-Permeable Membranes (AREA)
  • Separation By Low-Temperature Treatments (AREA)
  • Production Of Liquid Hydrocarbon Mixture For Refining Petroleum (AREA)
  • Degasification And Air Bubble Elimination (AREA)
EP93107550A 1988-11-15 1989-11-14 Verfahren zur gleichzeitigen Ausscheidung von CO2 und Benzin aus Methan, C2 und höheren Kohlenwasserstoffen und CO2 enthaltenden gasförmigen Kohlenwasserstoffen Expired - Lifetime EP0556875B1 (de)

Applications Claiming Priority (3)

Application Number Priority Date Filing Date Title
FR888814784A FR2641542B1 (fr) 1988-11-15 1988-11-15 Procede de decarbonatation et de degazolinage simultanes d'un melange gazeux constitue principalement d'hydrocarbures consistant en methane et hydrocarbures en c2 et plus et renfermant egalement co2
FR8814784 1988-11-15
EP89403123A EP0373983B1 (de) 1988-11-15 1989-11-14 Verfahren zur gleichzeitigen Ausscheidung von CO2 und Bearin aus Methan, C2 und höheren Kohlenwasserstoffen und CO2 enthatenden gasförmigen Kohlenwasserstoffen

Related Parent Applications (1)

Application Number Title Priority Date Filing Date
EP89403123.6 Division 1989-11-14

Publications (3)

Publication Number Publication Date
EP0556875A2 true EP0556875A2 (de) 1993-08-25
EP0556875A3 EP0556875A3 (en) 1993-11-10
EP0556875B1 EP0556875B1 (de) 1995-07-12

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Application Number Title Priority Date Filing Date
EP89403123A Expired - Lifetime EP0373983B1 (de) 1988-11-15 1989-11-14 Verfahren zur gleichzeitigen Ausscheidung von CO2 und Bearin aus Methan, C2 und höheren Kohlenwasserstoffen und CO2 enthatenden gasförmigen Kohlenwasserstoffen
EP93107550A Expired - Lifetime EP0556875B1 (de) 1988-11-15 1989-11-14 Verfahren zur gleichzeitigen Ausscheidung von CO2 und Benzin aus Methan, C2 und höheren Kohlenwasserstoffen und CO2 enthaltenden gasförmigen Kohlenwasserstoffen

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EP89403123A Expired - Lifetime EP0373983B1 (de) 1988-11-15 1989-11-14 Verfahren zur gleichzeitigen Ausscheidung von CO2 und Bearin aus Methan, C2 und höheren Kohlenwasserstoffen und CO2 enthatenden gasförmigen Kohlenwasserstoffen

Country Status (14)

Country Link
US (1) US5298156A (de)
EP (2) EP0373983B1 (de)
JP (1) JP2742328B2 (de)
AT (1) ATE124987T1 (de)
AU (1) AU627250B2 (de)
BR (1) BR8907193A (de)
CA (1) CA2002826C (de)
DE (2) DE68923459T2 (de)
ES (2) ES2050833T3 (de)
FR (1) FR2641542B1 (de)
NO (1) NO180687C (de)
RU (1) RU1836407C (de)
UA (1) UA26318A (de)
WO (1) WO1990005766A1 (de)

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NO302567B1 (no) * 1994-02-14 1998-03-23 Norsk Hydro As Mateanordning
FR2743083B1 (fr) * 1995-12-28 1998-01-30 Inst Francais Du Petrole Procede de deshydratation, de desacidification et de degazolinage d'un gaz naturel, utilisant un melange de solvants
JP5383338B2 (ja) * 2009-06-17 2014-01-08 三菱重工業株式会社 Ｃｏ２回収装置及びｃｏ２回収方法
GB201520405D0 (en) * 2015-11-19 2016-01-06 Isis Innovation Ltd And King Abdulaziz City For Science And Technology Hydrocarbon separation process

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Publication number Publication date
US5298156A (en) 1994-03-29
NO180687C (no) 1997-05-28
FR2641542B1 (fr) 1994-06-24
AU4637589A (en) 1990-06-12
EP0556875A3 (en) 1993-11-10
EP0556875B1 (de) 1995-07-12
FR2641542A1 (fr) 1990-07-13
BR8907193A (pt) 1991-03-05
NO903128L (no) 1990-09-11
AU627250B2 (en) 1992-08-20
JPH03503779A (ja) 1991-08-22
ATE124987T1 (de) 1995-07-15
NO903128D0 (no) 1990-07-13
CA2002826A1 (fr) 1990-05-15
JP2742328B2 (ja) 1998-04-22
ES2077452T3 (es) 1995-11-16
DE68923459D1 (de) 1995-08-17
DE68923459T2 (de) 1996-04-04
NO180687B (no) 1997-02-17
EP0373983A1 (de) 1990-06-20
EP0373983B1 (de) 1994-01-26
DE68912746D1 (de) 1994-03-10
UA26318A (uk) 1999-08-30
ES2050833T3 (es) 1994-06-01
CA2002826C (fr) 1999-06-29
DE68912746T2 (de) 1994-08-11
WO1990005766A1 (fr) 1990-05-31
RU1836407C (ru) 1993-08-23

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