EP0208609B1 - Verfahren und Einrichtung für das katalytische Kracken von Kohlenwasserstoffen mit Kontrolle der Reaktionstemperatur - Google Patents

Verfahren und Einrichtung für das katalytische Kracken von Kohlenwasserstoffen mit Kontrolle der Reaktionstemperatur Download PDF

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EP0208609B1
EP0208609B1 EP86401464A EP86401464A EP0208609B1 EP 0208609 B1 EP0208609 B1 EP 0208609B1 EP 86401464 A EP86401464 A EP 86401464A EP 86401464 A EP86401464 A EP 86401464A EP 0208609 B1 EP0208609 B1 EP 0208609B1
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Prior art keywords
catalyst
charge
temperature
injection
auxiliary fluid
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EP86401464A
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English (en)
French (fr)
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EP0208609B2 (de
EP0208609A1 (de
Inventor
Jean-Louis Mauleon
François Ville
Jean-Bernard Sigaud
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Total Marketing Services SA
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Total Raffinage Distribution SA
Compagnie de Raffinage et de Distribution Total France SA
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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
    • C10G11/00—Catalytic cracking, in the absence of hydrogen, of hydrocarbon oils
    • C10G11/14—Catalytic cracking, in the absence of hydrogen, of hydrocarbon oils with preheated moving solid catalysts
    • C10G11/18—Catalytic cracking, in the absence of hydrogen, of hydrocarbon oils with preheated moving solid catalysts according to the "fluidised-bed" technique
    • C10G11/187—Controlling or regulating
    • 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
    • C10G11/00—Catalytic cracking, in the absence of hydrogen, of hydrocarbon oils
    • C10G11/14—Catalytic cracking, in the absence of hydrogen, of hydrocarbon oils with preheated moving solid catalysts
    • C10G11/18—Catalytic cracking, in the absence of hydrogen, of hydrocarbon oils with preheated moving solid catalysts according to the "fluidised-bed" technique
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y10—TECHNICAL SUBJECTS COVERED BY FORMER USPC
    • Y10S—TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y10S208/00—Mineral oils: processes and products
    • Y10S208/01—Automatic control

Definitions

  • the present invention relates to catalytic cracking of hydrocarbon charges in a fluidized bed. It relates more particularly to a process and a device for such a catalytic cracking, with a regulation of the reaction temperature by quenching of the reaction products.
  • the catalyst of the FCC process and the feedstock to be treated are brought into contact at the base of a reactor made up of a column known as a "load lift", which techniques often designate by the English term “riser”. .
  • a load lift which techniques often designate by the English term “riser”.
  • At the top of the column is an enclosure concentric with the elevator.
  • a ballistic separation system to recover the catalyst entrained with the vapors.
  • Cyclonic systems are generally used.
  • the charge is discharged at the top of said enclosure, while the catalyst particles deactivated by coke deposition are collected at the base of the enclosure and meet there a stripping fluid such as water vapor, injected at the base from said enclosure, before being evacuated to a regenerator, in order to restore their activity by burning coke.
  • Combustion air is injected at the base of the regenerator, while at the top of the latter are provided cyclones making it possible to separate the combustion gas from the entrained particles of the regenerated catalyst.
  • This is evacuated to the bottom of the regenerator and recycled to the base of the elevator or "riser", where the charge is usually injected at a temperature between 80 ° C and 400 ° C and under a pressure ranging from 0 , 7 '10 5 3,5'105 relative Pascals.
  • the pair “charge preheating temperature / regenerated catalyst circulation” is therefore adjusted so as to determine the reaction temperature in any reaction zone, and in particular at the outlet of the riser.
  • the catalyst can be introduced with the feedstock at the top of an essentially descending or “dropper” reaction column, at the base of which the spent catalyst is recovered, stripped and sent to regeneration.
  • US-A-3,896,024 describes a process for catalytic cracking of a charge whose boiling point is between 650 and 720 ° F (343 and 382 ° C).
  • the charge is brought into contact with the catalyst in a rising flow column where the temperature of the mixture can reach at most 1000 ° F (538 ° C).
  • the charge is thermally cracked into fractions of lower boiling points.
  • a charge of preheated gas oil is injected into the column to lower the temperature of the reaction mixture between 800 and 900 ° F (426 and 482 ° C).
  • the mixture obtained is then catalytically cracked under milder conditions in the upper part of the column.
  • Petroleum charges characterized in that at least 10% of their weight has a boiling point above 500 ° C., have thus been able to be treated in the catalytic cracking units, by virtue of an increase in the temperature in the zone of injecting the catalyst and of the charge to be cracked (or “mixing zone”) and of a good spraying of the charge in this zone.
  • the heterogeneity of temperatures which results from such an injection, necessitated the development of reactors with short residence times, in order to avoid the occurrence of overcracking or of secondary reactions, such as polymerization reactions of cracked products, as well as to avoid the production of an excess of gases which are difficult to recover.
  • the temperature regulation carried out according to the invention therefore makes it possible to control the duration of the contact between the molecules to be catalytically cracked and the catalyst, and thus to avoid an excessive prolongation of the thermocracking generating coke and light gases, as well as the occurrence of side reactions linked to an unsuitable catalytic cracking temperature.
  • An object of the present invention is, therefore, in a process for catalytic cracking of a charge of hydrocarbons in a fluidized bed, to bring the charge and the catalyst into contact at a high temperature capable of preventing deposits of coke on the catalyst and optimally promote catalytic cracking of this charge.
  • Another object of the invention is to control the duration of contact of the catalyst and of the charge at this high temperature, so as to reduce the secondary reactions or to limit the thermocracking liable to occur.
  • the subject of the invention is therefore a process for catalytic cracking in a dilute fluidized bed and with a short contact time of a heavy hydrocarbon charge of which more than 10% by weight has a boiling point above 500 ° C., this process comprising a contacting phase, with ascending or descending flow, in a column, under cracking conditions, of said charge and of particles of a cracking catalyst, a phase of separation of the spent catalyst and of the charge cracked downstream of the injection zone of said charge with at least one stripping phase of the spent catalyst using a fluid, then a regeneration phase of said catalyst under conditions of combustion of the coke deposited on it , and finally a phase of recycling the regenerated catalyst to the supply of said column, this process being characterized in that injected into said column of regenerated catalyst under conditions such as the equilibrium temperature resulting from the melan ge of the vaporized charge and of the catalyst is at least greater than 500 ° C.
  • the injected fluid may be a liquid or a gas and, in particular, water, water vapor, or any hydrocarbon vaporizable under the injection conditions, in particular, coking or visbreaking gas oils. , catalytic thinners, heavy aromatic solvents, as well as certain deasphalting cuts extracted with heavy solvent.
  • this fluid will therefore have a selective quenching effect on the reaction mixture constituted by the charge and the grains of catalyst, and the injection rate of said fluid must be such that it makes it possible to regulate, under optimum conditions, the temperature of the catalytic cracking reaction, without harming the subsequent stripping of the spent catalyst and without causing condensation on the catalyst particles of the heaviest hydrocarbons present, which would result in an increased deposition of coke on the catalyst.
  • the conditions for injecting the fluid will be such that it causes an instantaneous lowering of the temperature of the reaction mixture of the order of 10 to 70 ° C., which, at constant final reaction temperature, therefore results in a substantially equivalent increase in the mixing temperature between the charge to be cracked and the regenerated catalyst grains.
  • the quenching carried out using the auxiliary fluid will take place less than a second after the injection of the cracked charge and , preferably, less than half a second after this.
  • the process according to the invention can be implemented both in a cracking column with ascending flow (riser, also called “riser”) and in a column with downward flow (“dropper”).
  • An important advantage of the process according to the invention is that it makes it possible to limit the catalyst regeneration temperature, due to a reduced deposition of coke, and makes it possible to convert heavy charges normally excluded in the catalytic cracking process into fluidized bed.
  • the conditions for injecting the charge and the catalyst will be such that the mixing temperature will be slightly higher than the vaporization temperature of the charge.
  • the conditions of injection of the auxiliary quenching fluid in particular, the flow rate, the temperature and the pressure, will have to be adjusted as a function of the characteristics of the charge and of the catalyst, as well as of the conditions of reaction of catalytic cracking and of profile of the desired temperature, that is to say in practice as a function of the mixing temperature and of the desired final reaction temperature.
  • a preferred embodiment of the process according to the invention therefore consists in regulating the injection of said auxiliary fluid into the cracking column so that the reaction temperature which results from this injection is maintained at a value predetermined and constant, but high enough that the effectiveness of the stripping is not substantially impaired.
  • the invention also relates to a catalytic cracking device for heavy loads of hydrocarbons of which more than 10% by weight have a boiling point above 500 ° C., comprising a cracking column with rising or falling flow, means for supplying said column under pressure with a hydrocarbon feedstock and particles of a regenerated cracking catalyst, a means for separating the products from the cracked feedstock and spent catalyst particles, at least one stripping means with at least one fluid from the spent catalyst particles, at least one unit for regenerating said catalyst by combustion of the coke deposited thereon, means for recycling the regenerated catalyst to said supply means and, downstream of the mixing zone in said column of the charge of hydrocarbons and particles of regenerated catalyst, at least one means for injecting an auxiliary fluid under flow, temperature and pressure conditions, such as the injection of this auxiliary fluid decreases the temperature of the reaction zone located immediately downstream independently of the mixing temperature, this device being characterized in that it comprises means for regulating the flow rate of said auxiliary fluid so that the temperature of the reaction zone downstream of the injection of the
  • this device will also include means for increasing the flow rate of the hot catalyst when the final reaction temperature tends to decrease compared to the set value.
  • the means for injecting an auxiliary fluid may advantageously be located in the reaction zone at a distance which may be between 0.1 and 0.8 times the length of said reaction zone and, preferably, between 0.1 and 0.5 times this length, downstream of the injection site of the load to be cracked.
  • This or these injection means will advantageously consist of an injection device of a type known per se, making it possible to distribute the fluid homogeneously over the entire section of the reaction zone.
  • the quantities necessary for regulating the mixing temperature will be injected using a spraying device making it possible, in a manner known per se, to spray this liquid in the form very fine mist over the entire section of the reaction zone so as to obtain as instantaneous heat transfer as possible.
  • a spraying device making it possible, in a manner known per se, to spray this liquid in the form very fine mist over the entire section of the reaction zone so as to obtain as instantaneous heat transfer as possible.
  • the flow required to achieve an identical temperature increase will be from 100 to 700 liters of hydrocarbon per cubic meter of charge treated.
  • the regenerated catalyst is injected via a pipe 1 at the base of an ascending flow column 2 or “riser”, as well as a carrier gas injected at 3.
  • the charge of hydrocarbons to be treated is itself even injected in 4 at the base of the column and the hydrocarbons and the particles of the catalyst are in contact in zone 2, immediately downstream of the injection of the feed.
  • the temperature of the catalyst + vaporized charge mixture is between approximately 500 and 650 ° C., depending on the nature of the charge and the desired conversion objectives.
  • an enclosure 6 for separating the cracked products and the spent catalyst particles.
  • injectors 7 of a stripping fluid generally steam, acting against the current of the separated catalyst particles.
  • the catalyst particles are removed at 8 to a second stripping device or to a regenerator, while the cracked products are removed at the upper part (not shown) of the enclosure 6.
  • an auxiliary fluid for quenching the cracked products is injected at 9 into part 5 of column 2, downstream of the contact zone between catalyst particles and vaporized charge.
  • This auxiliary fluid - water, water vapor, hydrocarbons, or other - is injected at a rate such that it lowers from 10 to 70 ° C, depending on the desired result, the temperature of the mixture, in order to optimize the reactions catalytic cracking of the charge.
  • the final temperature of the reaction zone thus cooled may be, for example, of the order of 500 ° C, but must be higher than the dew point of the heaviest hydrocarbons present.
  • a temperature probe 10 will be provided inside the enclosure 6 to measure the temperature there and to possibly control the valve 12 controlling the flow of the auxiliary fluid in the supply line 13 of the injection means. 9, so that the temperature in the enclosure 6 is maintained above a set temperature specific to the type of load treated.
  • the cracking column 20 is of the so-called “dropper” type, that is to say that the particles of regenerated catalyst 21 are injected into the upper part of the column 20 and fall there by gravity .
  • the charge to be cracked is also introduced into the upper part of the column at 22.
  • An enclosure 23 located at the base of the column 20 makes it possible to separate and evacuate the effluents, namely the products of cracking through the pipe 24, and the spent catalyst particles towards the base of this enclosure 23, in order to strike them, then convey them to the regeneration.
  • an auxiliary quenching fluid for the cracked products is injected at 26, downstream of the means 22 for injecting the charge. Its flow rate is such that, for a given mixing temperature, it lowers the final reaction temperature by approximately 10 to 70 ° C, to allow the catalytic cracking reactions to be carried out under optimal conditions.
  • a temperature probe 27, disposed before the pipe 24, makes it possible to control, by a valve 29 arranged on the supply pipe 30, the flow of auxiliary fluid of the injection means 26, in such a way that the temperature recorded in 27 is constantly equal to or higher than a set temperature, while the probe makes it possible to act on the injection temperature in the reaction zone and on the regulation of the injection flow rate in 26.
  • the cracking column 2 is again of the riser type and the reference numerals designating the elements of the unit are the same as for those of FIG. 1.
  • This figure presents a simplified and particularly advantageous mode of regulation. , according to the present invention.
  • the auxiliary fluid is injected at 9, or when the injection volume is increased, the final temperature of the catalytic reaction, measured at 10, will tend to decrease compared to the desired setpoint for the corresponding charge.
  • the valve 16, acting on the flow of hot regenerated catalyst will immediately ensure an increase in the mixing temperature which, taking into account the flow injected at 9, will make it possible to bring the final cracking temperature back to the set value.
  • the following two examples illustrate the advantages of the process according to the invention.
  • a commercial catalyst is used for cracking, comprising zeolites of high stability and a matrix capable of cracking - the heaviest hydrocarbon molecules under cracking conditions.
  • the table above shows the advantage resulting from raising the initial cracking temperature above 550 ° C and quenching the reaction products, using water, to bring the temperature down. of the mixture at 525 ° C.
  • the auxiliary fluid this time consists of a recycling of cracking effluents with a boiling point of between 340 ° C. and 460 ° C., carried out 0.2 seconds after injection of the charge into the mixing zone.
  • the operating conditions are as follows:
  • the heavy load considered could not have been treated without resorting to the means used in the present invention, insofar as, according to the prior art, at least 15% by weight of this load could not have been be vaporized, which would have led to a production of coke outside the limits compatible with the satisfaction of the thermal balance of the unit.
  • the mixing temperature was increased by approximately 40 ° C to ensure complete vaporization and the thermal shock conditions necessary for cracking the heaviest compounds present in this charge, after which the spraying of a hydrocarbon in the reaction medium makes it possible to reduce the final temperature to 510 ° C. and thus to ensure optimal conversion.
  • the process according to the invention therefore makes it possible to improve the performance of a cracking unit for a determined charge of hydrocarbons. It can advantageously be used to treat heavier and more contaminated loads with greater efficiency. In the same way, this process presents an exceptional attraction for the treatment of nitrogenous charges, or rich in polar compounds (resins, asphaltenes), where the strong presence of aromatic nitrogen is responsible for a spectacular fall of the conversion.
  • the conversion gain with the process according to the invention is of the order of 5.5% by volume. This is explained by the higher mixing temperature, which favorably displaces the adsorption balance of aromatic nitrogen, thereby reducing the neutralization of certain acid sites of the catalyst.

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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)
  • Production Of Liquid Hydrocarbon Mixture For Refining Petroleum (AREA)
  • Catalysts (AREA)

Claims (11)

1. Verfahren für das katalytische Kracken einer schweren Charge von Kohlenwasserstoffen, von der mehr als 10 Gew.-% einen Siedepunkt höher als 500°C aufweisen, mit
einer Phase, in welcher die Charge und Teilchen eines Krackkatalysators in verdünnter Wirbelschicht und mit kurzer Kontaktzeit im steigenden oder fallenden Strom in einer Kolonne unter Krackbedingungen miteinander in Berührung gebracht werden,
einer Phase hinter der Chargenspritzzone, in welcher gebrauchter Katalysator und die gekrackte Charge voneinander getrennt werden,
mindestens einer Phase, in welcher der gebrauchte Katalysator gestrippt wird,
danach einer Phase, in welcher der Katalysator unter Bedingungen regeneriert wird, bei denen der auf ihm abgelagerte Koks verbrennt, und
schließlich einer Phase, in welcher der regenerierte Katalysator zur Speisung der Kolonne rückgeführt wird, dadurch gekennzeichnet, daß
in die Kolonne regenerierter Katalysator unter solchen Bedingungen eingeblasen wird, daß die sich aus der gegenseitigen Vermischung der verdampften Charge und des Katalysators ergebende Beharrungstemperatur mindestens höher als 500°C und wenigstens um 40 bis 100°C höher als die Reaktionsendtemperatur am Kolonnenende ist, und
hinter dieser Vermischungszone, aber vor der Trennungsphase, ein Hilfsströmungsmittel unter solchen Bedingungen eingeblasen bzw. eingespritzt wird, daß das Einblasen bzw. Einspritzen dieses Hilfsströmungsmittels es der katalytischen Krackreaktion ermöglicht, sich unter milderen und von der Vermischungstemperatur unabhängigen Bedingungen zu vollziehen, wobei die Reaktionstemperatur jedoch über dem Taupunkt der schwersten vorhandenen Kohlenwasserstoffe liegt.
2. Verfahren nach Anspruch 1, dadurch gekennzeichnet, daß das Hilfsströmungsmittel mittels einer oder mehrerer Zerstäubungsvorrichtungen homogen über den gesamten Querschnitt der Reaktionszone eingeblasen bzw. eingespritzt wird.
3. Verfahren nach Anspruch 1 oder 2, dadurch gekennzeichnet, daß die Hilfsströmungsmitteleinblas- bzw. -einspritzbedingungen so sind, daß die Vermischungstemperatur der verdampften Charge und der Katalysatorteilchen gegenüber derjenigen Temperatur um etwa 10 bis 70°C abgesenkt wird, welche sich aus dem gegenseitigen Inberührungbringen von Katalysator und der Charge ergibt.
4. Verfahren nach Anspruch 1, 2 oder 3, dadurch gekennzeichnet, daß das Mittel zum Einblasen bzw. Einspritzen von Hilfsströmungsmittel, welches die Temperatur zu regeln erlaubt, in einem solchen Abstand angeordnet ist, daß die sich daraus ergebende Temperaturabsenkung weniger als eine Sekunde nach dem Einspritzen der Charge und vorzugsweise weniger als eine halbe Sekunde nach diesem Einspritzen stattfindet.
5. Verfahren nach Anspruch 1, 2, 3 oder 4, dadurch gekennzeichnet, daß es sich bei dem Hilfsströmungsmittel um Wasser oder Wasserdampf handelt.
6. Verfahren nach Anspruch 5, dadurch gekennzeichnet, daß das Wasser in einer Menge zwischen 20 und 150 1 je m3 an in die Reaktionszone eingespritzter Charge eingespritzt wird.
7. Verfahren nach einem der Ansprüche 1 bis 4, dadurch gekennzeichnet, daß es sich bei dem Hilfsströmungsmittel um einen bei den Einspritzbedingungen verdampfbaren Kohlenwasserstoff handelt, insbesondere ein Gasöl, ein katalytisches Verdünnungsmittel, ein schweres aromatisches Lösungsmittel oder eine mit schwerem Lösungsmittel extrahierte Entasphaltierungsfraktion.
8. Verfahren nach Anspruch 7, dadurch gekennzeichnet, daß der Kohlenwasserstoff in einer Menge zwischen 100 und 700 I je Kubikmeter an behandelter Charge eingespritzt wird.
9. Verfahren nach einem der vorstehenden Ansprüche, dadurch gekennzeichnet, daß die sich aus dem Einspritzen der zu krackenden Charge ergebende Vermischungstemperatur zwischen 500 und 650°C liegt.
10. Einrichtung für das katalytische Kracken von schweren Chargen von Kohlenwasserstoffen, von denen mehr als 10 Gew.-% einen Siedepunkt höher als 500°C aufweisen, mit
einer Krackkolonne (2; 20) mit steigendem oder fallendem Strom,
Mitteln (4, 22; 1,26) zum Speisen der Kolonne unter Druck mit einer Charge von Kohlenwasserstoffen und Teilchen eines regenerierten Krackkatalysators,
einem Mittel zum Trennen der Produkte der gekrackten Charge und der Teilchen gebrauchten Katalysators,
mindestens einem Mittel (7) zum Strippen der Teilchen gebrauchten Katalysators mit wenigstens einem Strömungsmittel,
mindestens einer Einheit zum Regenerieren des Katalysators durch Verbrennung des auf ihm abgelagerten Kokses,
Mitteln zum Rückführen des regenerierten Katalysators zu den Speisemitteln und
hinter der Zone zum gegenseitigen Vermischen der Charge von Kohlenwasserstoffen und der Teilchen des regenerierten Katalysators in der Kolonne,
mindestens einem Mittel (9; 26) zum Einblasen bzw. Einspritzen eines Hilfsströmungsmittels unter solchen Durchsatz-, Temperatur- und Druckbedingungen, daß das Einblasen bzw. Einspritzen dieses Hilfsströmungsmittels die Temperatur der unmittelbar dahinter angeordneten Reaktionszone unabhängig von der Vermischungstemperatur vermindert, gekennzeichnet durch
Mittel (10, 11 12; 27, 28, 29) zum Regeln des Hilfsströmungsmitteldurchsatzes derart, daß die Temperatur der Reaktionszone hinter dem Einblasen bzw. Einspritzen des Hilfsströmungsmittels auf einem der Art der zu krackenden Charge, dem verwendeten Katalysatortyp und der Art seiner Regenerierung entsprechenden Sollwert gehalten bleibt.
11. Einrichtung nach Anspruch 10, gekennzeichnet durch Mittel (15, 16) zur Erhöhung des Durchsatzes an heißem Katalysator, sobald die Reaktionsendtemperatur dahin tendiert, gegenüber dem Sollwert abzufallen.
EP86401464A 1985-07-10 1986-07-02 Verfahren und Einrichtung für das katalytische Kracken von Kohlenwasserstoffen mit Kontrolle der Reaktionstemperatur Expired - Lifetime EP0208609B2 (de)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
FR8510569A FR2584732B1 (fr) 1985-07-10 1985-07-10 Procede et dispositif pour le craquage catalytique de charges d'hydrocarbures, avec controle de la temperature de reaction
FR8510569 1985-07-10

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EP0208609A1 EP0208609A1 (de) 1987-01-14
EP0208609B1 true EP0208609B1 (de) 1989-06-14
EP0208609B2 EP0208609B2 (de) 1995-08-16

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US (1) US4818372A (de)
EP (1) EP0208609B2 (de)
CN (1) CN1015374B (de)
AR (1) AR240172A1 (de)
AU (1) AU585035B2 (de)
CA (1) CA1272974A (de)
DE (1) DE3663953D1 (de)
FR (1) FR2584732B1 (de)
ZA (1) ZA865183B (de)

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Publication number Publication date
EP0208609B2 (de) 1995-08-16
US4818372A (en) 1989-04-04
DE3663953D1 (en) 1989-07-20
AU585035B2 (en) 1989-06-08
AU5988186A (en) 1987-01-15
CN1015374B (zh) 1992-02-05
EP0208609A1 (de) 1987-01-14
FR2584732A1 (fr) 1987-01-16
CN86104812A (zh) 1987-01-07
AR240172A1 (es) 1990-02-28
ZA865183B (en) 1987-03-25
CA1272974A (fr) 1990-08-21
FR2584732B1 (fr) 1988-08-19

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