EP0370910A1 - Krackverfahren von schweren Kohlenwasserstoff-Einsätzen und Vorrichtung zur Ausführung des Verfahrens - Google Patents
Krackverfahren von schweren Kohlenwasserstoff-Einsätzen und Vorrichtung zur Ausführung des Verfahrens Download PDFInfo
- Publication number
- EP0370910A1 EP0370910A1 EP89403235A EP89403235A EP0370910A1 EP 0370910 A1 EP0370910 A1 EP 0370910A1 EP 89403235 A EP89403235 A EP 89403235A EP 89403235 A EP89403235 A EP 89403235A EP 0370910 A1 EP0370910 A1 EP 0370910A1
- Authority
- EP
- European Patent Office
- Prior art keywords
- zone
- reaction
- temperature
- bed
- cracking
- 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.)
- Granted
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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
- C10G15/00—Cracking of hydrocarbon oils by electric means, electromagnetic or mechanical vibrations, by particle radiation or with gases superheated in electric arcs
- C10G15/12—Cracking of hydrocarbon oils by electric means, electromagnetic or mechanical vibrations, by particle radiation or with gases superheated in electric arcs with gases superheated in an electric arc, e.g. plasma
-
- 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
- C10G47/00—Cracking of hydrocarbon oils, in the presence of hydrogen or hydrogen- generating compounds, to obtain lower boiling fractions
- C10G47/24—Cracking of hydrocarbon oils, in the presence of hydrogen or hydrogen- generating compounds, to obtain lower boiling fractions with moving solid particles
- C10G47/30—Cracking of hydrocarbon oils, in the presence of hydrogen or hydrogen- generating compounds, to obtain lower boiling fractions with moving solid particles according to the "fluidised-bed" technique
Definitions
- the present invention relates to a process for cracking heavy hydrocarbons into lighter hydrocarbons and to a device for implementing this process.
- the invention finds particular application in the chemical and energy industries.
- the object of the present invention is a process for cracking heavy hydrocarbons into lighter hydrocarbons which does not have the drawbacks of the prior techniques and which moreover makes it possible to obtain a selectivity in light hydrocarbons which is higher and with better yields.
- the process of the present invention consists in creating in a reaction chamber a bed of advantageously catalytic particles fluidized by a gaseous fluidization stream and in introducing a plasma jet preferably containing argon into the reaction chamber. , the jet being directed towards a determined place of the bed, so as to create a zone of high temperature constituting the reaction zone of higher temperature; consists in introducing a charge of heavy hydrocarbons in a place in the fluidized bed distant from the plasma jet to obtain the reaction zone of lower temperature and in introducing into the zone of higher temperature a light alkane, such as methane, or a mixing of light alkanes to effect the cracking of said heavy hydrocarbons in the fluidized bed, the latter quenching the reaction medium and catalyzing the cracking; and to evacuate the lighter hydrocarbons thus obtained, downstream of the zone of lower temperature.
- a light alkane such as methane, or a mixing of light alkanes
- the plasma is introduced at the periphery of the fluidized bed; A determined residence time is imposed on the products obtained in an area downstream from that of lower temperature; The flow rate of the fluidizing gas stream is determined to create a gushing fluidized bed;
- the fluidizing gas stream comprises at least argon and / or hydrogen;
- the plasma contains at least 80% by volume of argon and may additionally contain hydrogen;
- the plasma and the heavy hydrocarbons are introduced on either side of the gushing fluidized bed;
- the higher temperature reaction zone is at a temperature between about 5000 ° and 1000 ° C;
- the lower temperature zone is at a temperature between about 900 ° C and 500 ° C; Methane is introduced into the reaction zone, the temperature of which is between approximately 5000 ° C and 1000 ° C;
- the charge of heavy hydrocarbons is introduced into the fluidized bed gushing into the reaction zone, the temperature of which is between approximately 900 ° C. and 500 ° C.
- the fluidizing gas is preheated upstream of the fluidized bed to a temperature between 50 ° C and 500 ° C, preferably between 150 ° C and 350 ° C;
- the charge of heavy hydrocarbons is preheated and vaporized in the reaction chamber;
- the bed consists of particles of a refractory material chosen in particular from the group consisting of oxides, carbides, nitrides and borides; The particles in the bed have a catalytic effect;
- the bed also contains a catalyst;
- the cracking reaction is continued downstream of the lower temperature zone of the fluidized bed in a area with a temperature between about 650 ° C and 550 ° C.
- the present invention also relates to a device for implementing the above process, this device comprising a reaction chamber 1 comprising a bed of particles 2, means for injecting a gaseous stream of fluidization 3 of the bed located at the bottom of the chamber to produce a gushing fluidized bed, a plasma torch 6 preferably containing argon and adapted to inject the plasma in the reaction chamber towards the fluidized bed to create at least two reaction zones of different temperatures and determining a higher temperature reaction zone and a lower temperature zone, means 4 for introducing the charge of heavy hydrocarbons located at the lower temperature reaction zone, means for introducing 5 of a light alkane, such as methane, or of a mixture of light alkanes in the higher temperature zone and means 7 intended to continue the reaction. cracking and to evacuate the lighter hydrocarbons thus obtained.
- the plasma torch 6 and the means for introducing heavy hydrocarbons 4 are arranged on either side of the gushing fluidized bed;
- the means for introducing the charge of heavy hydrocarbons consist of an injection pipe or the like;
- the means for introducing the light alkane, such as methane, or the mixture of light alkanes are constituted by an injection pipe or the like;
- the means 7 for continuing the cracking reaction and for removing the hydrocarbons obtained consist for example of a tubular reactor;
- the reaction chamber has a cylindrical, parallelepipedic, spherical or similar shape;
- the plasma torch is preferably connected at a side wall of the chamber so that the plasma is injected laterally into the fluidized bed;
- the walls of the reaction chamber are preferably made of a refractory material such as alumina;
- the bottom 8 of the reaction chamber has an upwardly flared shape at the bottom of which open means 9 for injecting the fluidizing gas.
- FIG. 1 represents a preferred embodiment of the method and the device of the invention
- FIG. 2 represents a curve illustrating the influence of the methane flow rate on the cracking rate, d (l / min), signifying the CH4 flow rate and% signifying the cracking rate.
- the method of the invention is implemented using a device of the type shown in FIG. 1 and comprising a reaction chamber 1 having for example the general shape of a rectangular parallelepiped whose bottom 8 has an upward flared shape and connected at its lower part to means 3 for injecting a gaseous fluidization stream, and containing a mass of particles of a material intended to form a fluidized bed 2, and a plasma torch 6 of a gas preferably containing argon, suitable for introducing the plasma inside the reaction chamber and towards the fluidized particle bed.
- the plasma torch 6 is connected at a side wall of the reaction chamber, so that the plasma is introduced laterally into the fluidized bed.
- a preferably tubular reactor 7 is connected to the upper part of the reaction chamber 1 so that the reactor 7 communicates with the interior of the reaction chamber.
- Means 4 for introducing the charge of heavy hydrocarbons are provided and connected to a wall of the reaction chamber 1 in such a way that the heavy hydrocarbons are brought into contact with the fluidized bed in an area of the reaction chamber having a determined temperature between about 900 ° C and 500 ° C.
- the injection means 4 may in particular comprise an injection rod or the like.
- Means 5 for injecting a light alkane, such as methane, or a mixture of light alkanes are provided and are connected at the bottom of the reaction chamber 1 so as to introduce the methane into the fluidized bed at a high temperature zone, between about 5000 ° C and 1000 ° C, of the reaction chamber 1.
- These introduction means 5 can be represented by an injection rod or the like.
- the reaction chamber 1 has internal walls by example in refractory alumina 4mm thick, externally insulated by a layer of porous bricks 20mm thick bonded with refractory cement on the alumina.
- the layer of bricks is itself covered by a layer of glass wool about 14 mm thick wrapped in a layer of asbestos.
- Thermocouples (not shown) are installed in the reaction chamber to measure the fluidized bed temperatures.
- the means 3 for injecting the gaseous fluidization stream comprise, for example, an opaque silica tube 9 with a length of approximately 300 mm and a diameter of approximately 40 mm opening at the bottom of the reaction chamber 1.
- the tube is surrounded by a 500 W heating tape (not shown) intended to preheat the fluidizing gas and it is lined with refractory balls with a diameter of approximately 2 to 6 mm favoring the heat exchanges between the gas and the wall of the tube.
- the lower part of the tube 9 is fitted with a brass injector 11.
- the tubular reactor 7 is for example constituted by a silica tube of approximately 85 mm in diameter and approximately 500 mm in length.
- Thermocouples (not shown) are installed in this tube to measure the temperature of the gas stream flowing therein.
- the outlet of this tube can be connected to a water heat exchanger (not shown) in which the reaction mixture is cooled before being taken for analysis.
- the plasma torch and the means for introducing heavy hydrocarbons are connected at the level of the reaction chamber so that the plasma and the heavy hydrocarbons are introduced on either side of the fluidized bed on the side opposite to the plasma torch. with respect to the jet of particles from the bed.
- the angle of introduction of the torch into the chamber is 20 ° relative to the horizontal section of the reaction chamber.
- this torch consists of two concentric tubes of silica, with an outside diameter of 30 mm, surrounded by five hollow inductive turns of water-cooled copper, traversed by an electric current at high frequency.
- the bed consists of particles of a material chosen in particular from the group consisting of oxides, carbides, nitrides and borides.
- oxides aluminum Al2O3 magnesium MgO calcium
- - carbides silicon SiC thorium ThC boron B4C - nitrides boron BN hafnium HfN zirconium ZrN - borides thorium ThB4 niobium NbB2 zirconium ZrB2.
- the particles of beds must be able to withstand high temperatures and because they are in contact with the plasma jet.
- the particles of the bed can themselves act as a catalyst and it is also possible to add another catalyst to them.
- the particles of the fluidized bed have a diameter of between approximately 250 and 400 ⁇ . The particle size chosen must allow a gushing fluidization without entraining the particles out of the reaction chamber 1.
- the mass of particles, of determined diameter, which may contain a catalyst, is made to fluidize into a gushing bed, having the shape of a fountain falling on the walls of the reaction chamber, by the constant flow of a fluidizing gas formed. argon or a mixture of argon and hydrogen.
- the fluidizing gas is preheated in the tube 9 which is lined with balls, for example of alumina.
- the plasma torch 6 injects a plasma of a gas preferably containing argon towards the fluidized bed of particles where an efficient transfer of heat takes place between the plasma and the fluidized bed.
- the injection rod 5 injects, for example, methane, inside the fluidized bed in an area close to that of the plasma injection and having a temperature between approximately 5000 ° C. and 1000 ° C. In this relatively high temperature zone, the methane will decompose as follows: CH4 ⁇ CH3 . + H. CH3 ⁇ CH2 . + H. etc ...
- Radicals favoring the cracking reaction of heavy hydrocarbons are therefore formed in this zone at relatively high temperature.
- the heavy hydrocarbon injection pipe 4 makes it possible to introduce them into the fluidized bed in a determined region having a temperature between approximately 900 ° C. and 500 ° C. and lying approximately opposite the plasma injection zone. .
- the methane will convert as described above inside the fluidized bed.
- the radicals thus formed will cross the fluidized bed in the direction of the zone of lower temperature at the level of which the charge of heavy hydrocarbons is introduced and will initiate the cracking reaction of the latter.
- the primary advantage of this type of device is that it makes it possible to use methane directly to promote cracking and for this purpose the device has a reaction space at two zones of different temperatures by means of the jet of particles which allows to separate the reaction space into these two zones.
- a fluidized bed of this type in the process of the present invention has significant advantages for the following reasons: - its heat transfer properties allow efficient quenching of the plasma; - Its viscosity substantially equal to that of the plasma ensures a very good mixture between it and the fluidized bed; and - its possible catalytic properties can ensure the direct transformation of the reactants to be converted.
- the methane will be converted in the fluidized bed in a region close to the plasma injection and in which the quenching carried out by the fluidized bed makes it possible to have a temperature suitable for the transformation of methane into radicals.
- These radicals from the higher temperature zone will favor the cracking reaction of heavy hydrocarbons at a temperature lower than that of the higher temperature zone, while avoiding the formation of carbon black.
- the reaction for converting heavy hydrocarbons into lighter hydrocarbons will continue in an area located downstream from the lower temperature area of the fluidized bed.
- a temperature gradient is created from the region downstream from the fluidized bed to the tubular reactor 7 varying from about 650 ° C to 550 ° C and thus allowing the completion of the cracking reaction.
- an aliphatic C16 hydrocarbon was treated at a rate of about 14 to 25 g / minute to carry out the cracking reaction and the products were analyzed by chromatography using a flame ionization detector equipped with a 10% SE 30 column for the separation of liquid hydrocarbons and a 7% squalane column for the separation of gaseous and light hydrocarbons.
- the plasma torch operates at a frequency of 5 MHz for an actual power of 2.38 kW.
- the injection angle is 20 °.
- the plasma gases introduced are argon at a flow rate of 27 l / min and hydrogen at a flow rate of 6 l / min.
- the bed is made up of alumina particles (650g) with a mean diameter of 300 ⁇ .
- the particles of the bed are fluidized by a mixture of argon at a flow rate of 10 l / min and hydrogen at a flow rate of 14 l / min.
- the fluidizing gases are preheated to a temperature between 50 ° C and 500 ° C, preferably between 150 ° C and 350 ° C.
- the average cracking temperature is 727 ° C.
- Methane is introduced at a flow rate of 1 l / min.
- the plasma torch operates at a frequency of 5 MHz for an actual power of 2.52 kW.
- the injection angle is 20 °.
- the plasma gases introduced are argon, at a flow rate of 27 l / min and hydrogen at a flow rate of 6 l / min.
- the bed is made up of alumina particles (650g) with a mean diameter of 300 ⁇ .
- the particles of the bed are put in fluidization with a mixture of argon, at a flow rate of 10 l / min and of hydrogen at a flow rate of 14 l / min.
- the fluidizing gases are preheated to a temperature between 50 and 500 ° C, preferably between 150 ° C and 350 ° C.
- the average cracking temperature is 730 ° C.
- Methane is introduced at a flow rate of 0.46 l / min.
- the plasma torch operates at a frequency of 5 MHz for an actual power of 2.45 kW.
- the injection angle is 20 °.
- the plasma gases introduced are argon, at a flow rate of 27 l / min and hydrogen at a flow rate of 6 l / min.
- the bed is made up of alumina particles (650g) with a mean diameter of 300 ⁇ .
- the particles of the bed are fluidized by a mixture of argon at a flow rate of 10 l / min and hydrogen at a flow rate of 14 l / min.
- the fluidizing gases are preheated to a temperature between 50 and 100 ° C, preferably between 150 ° C and 350 ° C.
- the average cracking temperature is 725 ° C.
- Methane is introduced at a flow rate of 0.15 l / min.
- the plasma torch operates at a frequency of 5 MHz for an actual power of 2.45 kW.
- the injection angle is 20 °.
- the plasma gases introduced are argon at a flow rate of 27 l / min and hydrogen at a flow rate of 6 l / min.
- the bed is made up of alumina particles (650g) with a mean diameter of 300 ⁇ .
- the particles of the bed are fluidized by a mixture of argon at a flow rate of 10 l / min and hydrogen at a flow rate of 14 l / min.
- the fluidizing gases are preheated to a temperature between 50 and 500 ° C, preferably between 150 ° C and 300 ° C.
- the average cracking temperature is 720 ° C. We does not inject methane.
- FIG. 2 shows the evolution of the cracking rate as a function of the methane flow rate.
- BOARD products (g) / 100 g cracked cracking rate (%)
- the method and the device of the present invention allow rigorous control of the temperature in the cracking zone by the combined effects of the electric power supplied to the plasma, the angle of injection of the plasma, the flow rate of hydrocarbons. heavy and the fluidization gas flow.
- the plasma used can be produced in any way, in particular by blown, transferred electric arc or even by induction.
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- Chemical & Material Sciences (AREA)
- Engineering & Computer Science (AREA)
- Oil, Petroleum & Natural Gas (AREA)
- Organic Chemistry (AREA)
- Chemical Kinetics & Catalysis (AREA)
- General Chemical & Material Sciences (AREA)
- Physics & Mathematics (AREA)
- Mechanical Engineering (AREA)
- Electromagnetism (AREA)
- Plasma & Fusion (AREA)
- Production Of Liquid Hydrocarbon Mixture For Refining Petroleum (AREA)
- Hydrogen, Water And Hydrids (AREA)
- Devices And Processes Conducted In The Presence Of Fluids And Solid Particles (AREA)
- Organic Low-Molecular-Weight Compounds And Preparation Thereof (AREA)
- Treatment Of Steel In Its Molten State (AREA)
Priority Applications (1)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
AT89403235T ATE78287T1 (de) | 1988-11-24 | 1989-11-22 | Krackverfahren von schweren kohlenwasserstoffeins|tzen und vorrichtung zur ausfuehrung des verfahrens. |
Applications Claiming Priority (2)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
FR8815363 | 1988-11-24 | ||
FR8815363A FR2639354B1 (fr) | 1988-11-24 | 1988-11-24 | Procede de craquage d'une charge d'hydrocarbures lourds en hydrocarbures plus legers et dispositif pour la mise en oeuvre de ce procede |
Publications (2)
Publication Number | Publication Date |
---|---|
EP0370910A1 true EP0370910A1 (de) | 1990-05-30 |
EP0370910B1 EP0370910B1 (de) | 1992-07-15 |
Family
ID=9372213
Family Applications (1)
Application Number | Title | Priority Date | Filing Date |
---|---|---|---|
EP89403235A Expired - Lifetime EP0370910B1 (de) | 1988-11-24 | 1989-11-22 | Krackverfahren von schweren Kohlenwasserstoff-Einsätzen und Vorrichtung zur Ausführung des Verfahrens |
Country Status (11)
Country | Link |
---|---|
US (1) | US5026949A (de) |
EP (1) | EP0370910B1 (de) |
AT (1) | ATE78287T1 (de) |
AU (1) | AU627244B2 (de) |
CA (1) | CA2003619A1 (de) |
DE (1) | DE68902132T2 (de) |
ES (1) | ES2034717T3 (de) |
FR (1) | FR2639354B1 (de) |
GR (1) | GR3005786T3 (de) |
NO (1) | NO894672L (de) |
NZ (1) | NZ231496A (de) |
Cited By (1)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
US8192591B2 (en) | 2005-12-16 | 2012-06-05 | Petrobeam, Inc. | Self-sustaining cracking of hydrocarbons |
Families Citing this family (5)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
GB9216509D0 (en) * | 1992-08-04 | 1992-09-16 | Health Lab Service Board | Improvements in the conversion of chemical moieties |
EP0907354B1 (de) | 1996-03-14 | 2002-05-29 | Johnson & Johnson Consumer Companies, Inc. | Reinigende und feuchthaltende tensidzusammensetzungen |
US11021661B2 (en) * | 2012-02-21 | 2021-06-01 | Battelle Memorial Institute | Heavy fossil hydrocarbon conversion and upgrading using radio-frequency or microwave energy |
US9862892B2 (en) | 2012-02-21 | 2018-01-09 | Battelle Memorial Institute | Heavy fossil hydrocarbon conversion and upgrading using radio-frequency or microwave energy |
JP7158379B2 (ja) * | 2019-04-26 | 2022-10-21 | 株式会社Fuji | プラズマ処理装置 |
Citations (3)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
EP0120625A1 (de) * | 1983-03-02 | 1984-10-03 | The British Petroleum Company p.l.c. | Verfahren zur Umwandlung mit elektrischem Bogen und Apparat |
EP0292391A1 (de) * | 1987-05-22 | 1988-11-23 | Electricite De France | Hydrokrackverfahren von Kohlenwasserstoffen und Vorrichtung zur Ausführung des Verfahrens |
EP0316234A1 (de) * | 1987-11-10 | 1989-05-17 | Electricite De France | Verfahren und Einrichtung für die hydrierende Pyrolyse von schweren Kohlenwasserstoffen durch einen Plasmastrahl, insbesondere ein H2/CH4-Plasma |
-
1988
- 1988-11-24 FR FR8815363A patent/FR2639354B1/fr not_active Expired - Fee Related
-
1989
- 1989-11-22 US US07/440,300 patent/US5026949A/en not_active Expired - Fee Related
- 1989-11-22 EP EP89403235A patent/EP0370910B1/de not_active Expired - Lifetime
- 1989-11-22 CA CA002003619A patent/CA2003619A1/en not_active Abandoned
- 1989-11-22 AT AT89403235T patent/ATE78287T1/de active
- 1989-11-22 DE DE8989403235T patent/DE68902132T2/de not_active Expired - Fee Related
- 1989-11-22 ES ES198989403235T patent/ES2034717T3/es not_active Expired - Lifetime
- 1989-11-23 NO NO89894672A patent/NO894672L/no unknown
- 1989-11-23 AU AU45521/89A patent/AU627244B2/en not_active Ceased
- 1989-11-23 NZ NZ231496A patent/NZ231496A/en unknown
-
1992
- 1992-09-24 GR GR920402108T patent/GR3005786T3/el unknown
Patent Citations (3)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
EP0120625A1 (de) * | 1983-03-02 | 1984-10-03 | The British Petroleum Company p.l.c. | Verfahren zur Umwandlung mit elektrischem Bogen und Apparat |
EP0292391A1 (de) * | 1987-05-22 | 1988-11-23 | Electricite De France | Hydrokrackverfahren von Kohlenwasserstoffen und Vorrichtung zur Ausführung des Verfahrens |
EP0316234A1 (de) * | 1987-11-10 | 1989-05-17 | Electricite De France | Verfahren und Einrichtung für die hydrierende Pyrolyse von schweren Kohlenwasserstoffen durch einen Plasmastrahl, insbesondere ein H2/CH4-Plasma |
Cited By (2)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
US8192591B2 (en) | 2005-12-16 | 2012-06-05 | Petrobeam, Inc. | Self-sustaining cracking of hydrocarbons |
US8911617B2 (en) | 2005-12-16 | 2014-12-16 | Petrobeam, Inc. | Self-sustaining cracking of hydrocarbons |
Also Published As
Publication number | Publication date |
---|---|
FR2639354B1 (fr) | 1993-01-22 |
DE68902132T2 (de) | 1993-03-04 |
GR3005786T3 (de) | 1993-06-07 |
AU4552189A (en) | 1990-06-28 |
ATE78287T1 (de) | 1992-08-15 |
ES2034717T3 (es) | 1993-04-01 |
DE68902132D1 (de) | 1992-08-20 |
FR2639354A1 (fr) | 1990-05-25 |
AU627244B2 (en) | 1992-08-20 |
CA2003619A1 (en) | 1990-05-24 |
EP0370910B1 (de) | 1992-07-15 |
NZ231496A (en) | 1992-03-26 |
NO894672D0 (no) | 1989-11-23 |
US5026949A (en) | 1991-06-25 |
NO894672L (no) | 1990-05-25 |
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