EP0176920B1 - Aqueous coal dispersions - Google Patents
Aqueous coal dispersions Download PDFInfo
- Publication number
- EP0176920B1 EP0176920B1 EP85112061A EP85112061A EP0176920B1 EP 0176920 B1 EP0176920 B1 EP 0176920B1 EP 85112061 A EP85112061 A EP 85112061A EP 85112061 A EP85112061 A EP 85112061A EP 0176920 B1 EP0176920 B1 EP 0176920B1
- Authority
- EP
- European Patent Office
- Prior art keywords
- weight
- alcohol
- coal
- dispersions
- mixture
- 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 - Lifetime
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Classifications
-
- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10L—FUELS NOT OTHERWISE PROVIDED FOR; NATURAL GAS; SYNTHETIC NATURAL GAS OBTAINED BY PROCESSES NOT COVERED BY SUBCLASSES C10G, C10K; LIQUEFIED PETROLEUM GAS; ADDING MATERIALS TO FUELS OR FIRES TO REDUCE SMOKE OR UNDESIRABLE DEPOSITS OR TO FACILITATE SOOT REMOVAL; FIRELIGHTERS
- C10L1/00—Liquid carbonaceous fuels
- C10L1/32—Liquid carbonaceous fuels consisting of coal-oil suspensions or aqueous emulsions or oil emulsions
- C10L1/326—Coal-water suspensions
Definitions
- the invention relates to aqueous, optionally methanol-containing pumpable and flowable coal dispersions with a special, ethoxylated, straight-chain, saturated fatty alcohol mixture as a nonionic dispersant and the use of these dispersants in coal-water dispersions.
- Aqueous coal dispersions have become increasingly important in recent times, especially with regard to their cheap transportation options, e.g. B. in pipelines.
- aqueous carbon dispersions which contain higher molecular weight polyalkylene oxides as nonionic surface-active dispersants.
- polyalkylene oxides of alkylphenols such as nonylphenoxypolyethylene oxide with more than a hundred ethylene oxide units.
- PCT applications WO 83/04044 and WO 83/04047 generally show ethoxylated aliphatic alcohols with 10 to 24 carbon atoms and 40 to 200 ethylene oxide (EO) units for the preparation of aqueous carbon dispersions.
- EO ethylene oxide
- the solution described is not always sufficient for practical use: the disadvantage is the excessively high viscosity of the carbon dispersions produced with it.
- the object of the invention is to provide new dispersants for coal dispersions with different types of coal.
- the ethoxylation product thereof is a mixture of straight-chain, saturated primary fatty alcohols of the composition 0.3 to 0.7% by weight of C 12 alcohol, 3.0 to 5.0% by weight of C 14 alcohol, 25 to 35% by weight C 16 alcohol, 65 to 70% by weight C 18 alcohol and 0.5 to 3.0% by weight C 2 o alcohol with 190 to 220 ethylene oxide units are preferred.
- the mixture according to the invention achieves a substantially better effect with regard to a reduction in viscosity of the carbon dispersions produced therewith compared to the saturated fatty alcohols ethoxylated as individual compounds.
- the optimum found was in no way obvious.
- the coal dispersions according to the invention preferably contain a floated, ground coal with a suitable particle size distribution of less than 300 ⁇ m.
- coal with a high ash content is generally more difficult to disperse than coal with a low ash content.
- High ash content means approx. 8 to 12%, lower ash content less than 4% ash.
- the sulfur content of the preferably used floated coal is generally less than 1%.
- the pumpable and flowable properties relate to the viscosity of the coal dispersion.
- a dispersion with 2000 mPa.s is just barely flowable.
- the desired values are 1000 mPa.s and below.
- the optimally desired range can be specified with less than 800 mPa.s. As shown in the examples, it is easily achieved in the coal dispersions according to the invention.
- methanol As already mentioned, 1 to 60% by weight of the water can be replaced by methanol.
- the addition of methanol serves for the purpose of lowering the viscosity (pumpability) of the coal dispersions at temperatures below 0 ° C (e.g. to -20 ° C).
- the preparation of the dispersants to be used according to the invention is known per se and is carried out by the processes described.
- the degree of ethoxylation is based on the average molecular weight which results from the hydroxyl number of the mixture.
- aqueous coal dispersions according to the invention are prepared in a conventional manner.
- a concentrated aqueous solution which contains 40 to 70% by weight of the dispersant according to the invention and which, in contrast to some dispersants of the prior art, can be easily prepared, is added to the amount of water which, with vigorous stirring, the ground coal and optionally further additives are fed.
- A. Preparation of the Dispersants According to the Invention The alcohol mixture is mixed with 1% by weight of potassium hydroxide and reacted with ethylene oxide in portions at 120-130 ° C., the pressure not exceeding 10 bar.
- the starting material to be ethoxylated has the following composition:
- the viscosity of the dispersion [mPas] is determined using a rotary viscometer at 20 ° C. and a shear rate D of 220 s-.
- "not measurable” means a viscosity greater than 20,000.
- Comparative Examples 1 to 14 correspond to PCT application WO-8-304 044. They are not suitable for practical use.
- Examples 15 to 18 according to the invention are distinguished by superior viscosities.
- Examples 19 to 22 show that there is an optimization in the range according to the invention. A lower or higher degree of ethoxylation leads to higher viscosity values.
Description
Die Erfindung betrifft wäßrige, gegebenenfalls methanolhaltige pumpbare und fließfähige Kohledispersionen mit einem speziellen, ethoxylierten, geradkettigen, gesättigten Fettalkoholgemisch als nichtionischem Dispergiermittel sowie die Verwendung dieser Dispergiermittel in Kohle-Wasser-Dispersionen.The invention relates to aqueous, optionally methanol-containing pumpable and flowable coal dispersions with a special, ethoxylated, straight-chain, saturated fatty alcohol mixture as a nonionic dispersant and the use of these dispersants in coal-water dispersions.
Wäßrige Kohledispersionen haben in neuerer Zeit zunehmend an Bedeutung gewonnen, insbesondere im Hinblick auf ihre günstigen Transportmöglichkeiten, z. B. in Pipelines.Aqueous coal dispersions have become increasingly important in recent times, especially with regard to their cheap transportation options, e.g. B. in pipelines.
Aus der US-PS-4 358 293 sind wäßrige Kohledispersionen bekannt, die als nichtionische oberflächenaktive Dispergiermittel höhermolekulare Polyalkylenoxide enthalten. U. a. werden Polyalkylenoxide von Alkylphenolen, wie Nonylphenoxypolyethylenoxid mit mehr als hundert Ethylenoxideinheiten, beschrieben.From US Pat. No. 4,358,293, aqueous carbon dispersions are known which contain higher molecular weight polyalkylene oxides as nonionic surface-active dispersants. Among others describe polyalkylene oxides of alkylphenols, such as nonylphenoxypolyethylene oxide with more than a hundred ethylene oxide units.
Die verschiedenen Tenside erweisen sich bei der Anwendung nicht in allen Fällen als besonders gut geeignet, d. h. sie sind nicht für alle Kohlearten anwendbar. Weiterhin sind die bisher verwendeten Dispergiermittel teilweise schwierig zu handhaben, da sie u. U. in Wasser eine sehr langsame Lösungsgeschwindigkeit aufweisen und teilweise konzentrierte wäßrige Lösungen nicht herstellbar sind.The various surfactants do not prove to be particularly suitable in all cases, ie. H. they are not applicable to all types of coal. Furthermore, the dispersants used to date are sometimes difficult to handle because they u. U. have a very slow dissolution rate in water and partially concentrated aqueous solutions cannot be prepared.
Aus den PCT-Anmeldungen WO 83/04044 und WO 83/04047 gehen in allgemeiner Form ethoxylierte aliphatische Alkohole mit 10 bis 24 C-Atomen und 40 bis 200 Ethylenoxid (EO)-Einheiten für die Herstellung von wäßrigen Kohledispersionen hervor. Dabei sind für die bevorzugten Alkohole mit 10 bis 24 C-Atomen 40 bis 100 EO-Einheiten oder ein Verhältnis von EO-Einheiten zur Zahl der C-Atome von 3,5 bis 6,0, d. h. etwa 150 EO-Einheiten, bevorzugt. Aber auch hier ist die beschriebene Lösung nicht immer für die Praxis ausreichend: nachteilig ist insbesondere die zu hohe Viskosität der damit hergestellten Kohledispersionen.PCT applications WO 83/04044 and WO 83/04047 generally show ethoxylated aliphatic alcohols with 10 to 24 carbon atoms and 40 to 200 ethylene oxide (EO) units for the preparation of aqueous carbon dispersions. For the preferred alcohols having 10 to 24 carbon atoms, 40 to 100 EO units or a ratio of EO units to the number of carbon atoms is from 3.5 to 6.0, ie. H. about 150 EO units, preferred. But here, too, the solution described is not always sufficient for practical use: the disadvantage is the excessively high viscosity of the carbon dispersions produced with it.
Aufgabe der Erfindung ist es, neue Dispergiermittel für Kohledispersionen mit unterschiedlichen Kohletypen zur Verfügung zu stellen.The object of the invention is to provide new dispersants for coal dispersions with different types of coal.
Es wurde gefunden, daß spezielle, ethoxylierte geradkettige, gesättigte primäre Fettalkoholgemische hervorragend als Dispergiermittel für wäßrige Kohledispersionen geeignet sind.It has been found that special, ethoxylated, straight-chain, saturated primary fatty alcohol mixtures are outstandingly suitable as dispersants for aqueous carbon dispersions.
Gegenstand der Erfindung ist die Verwendung von Ethoxylierungsprodukten eines Gemisches von geradkettigen, gesättigten primären Fettalkoholen der Zusammensetzung
- 0,1 bis 2,0 Gew.-% C12-Alkohol,
- 3,0 bis 6,0 Gew.-% C14-Alkohol,
- 20,0 bis 35,0 Gew.-% C16-Alkohol,
- 55,0 bis 75,0 Gew.-% C18-Alkohol und
- 0,5 bis 3,0 Gew.-% C2o-A)kohoi
mit 180 bis 230 Ethylenoxideinheiten, bezogen auf das mittlere Molekulargewicht der Alkohole, als nichtionische Dispergiermittel in wäßrigen Kohlendispersionen in einer Menge von 0,1 bis 1,5 Gew.-% bezogen auf das Gesamtgewicht der Mischung.
- 0.1 to 2.0% by weight of C 12 alcohol,
- 3.0 to 6.0% by weight of C 14 alcohol,
- 20.0 to 35.0% by weight of C 16 alcohol,
- 55.0 to 75.0% by weight of C 18 alcohol and
- 0.5 to 3.0 wt .-% C 2 oA) kohoi
with 180 to 230 ethylene oxide units, based on the average molecular weight of the alcohols, as nonionic dispersants in aqueous carbon dispersions in an amount of 0.1 to 1.5% by weight, based on the total weight of the mixture.
Davon ist das Ethoxylierungsprodukt eines Gemisches von geradkettigen, gesättigten primären Fettalkoholen der Zusammensetzung 0,3 bis 0,7 Gew.% C12-Alkohol, 3,0 bis 5,0 Gew.% C14-Alkohol, 25 bis 35 Gew.% C16-Alkohol, 65 bis 70 Gew.% C18-Alkohol und 0,5 bis 3,0 Gew.% C2o-Alkohol mit 190 bis 220 Ethylenoxideinheiten bevorzugt.The ethoxylation product thereof is a mixture of straight-chain, saturated primary fatty alcohols of the composition 0.3 to 0.7% by weight of C 12 alcohol, 3.0 to 5.0% by weight of C 14 alcohol, 25 to 35% by weight C 16 alcohol, 65 to 70% by weight C 18 alcohol and 0.5 to 3.0% by weight C 2 o alcohol with 190 to 220 ethylene oxide units are preferred.
In überraschender und nicht vorhersehbarer Weise wird durch die erfindungsgemäße Mischung gegenüber den als Einzelverbindungen ethoxylierten gesättigten Fettalkohole eine wesentlich bessere Wirkung im Hinblick auf eine Viskosiätsreduzierung der damit hergestellten Kohledispersionen erreicht. Das gefundene Optimum hat in keiner Weise nahegelegen.In a surprising and unpredictable manner, the mixture according to the invention achieves a substantially better effect with regard to a reduction in viscosity of the carbon dispersions produced therewith compared to the saturated fatty alcohols ethoxylated as individual compounds. The optimum found was in no way obvious.
Die erfindungsgemäßen Kohledispersionen enthalten bevorzugt eine flotierte, gemahlene Kohle mit einer zweckmäßigen Korngrößenverteilung von kleiner 300 pm.The coal dispersions according to the invention preferably contain a floated, ground coal with a suitable particle size distribution of less than 300 μm.
Eine beispielhafte und besonders zweckmäßige Verteilung bedeutet 100 % kleiner 300 µm, 80 % kleiner 200 µm und 50 % kleiner 50 pm.An exemplary and particularly expedient distribution means 100% smaller than 300 µm, 80% smaller than 200 µm and 50% smaller than 50 pm.
Es ist selbstverständlich, daß Kohle mit einem hohen Aschegehalt in der Regel schwerer dispergiert werden kann als Kohle mit einem niederen Aschegehalt. Hoher Aschegehalt bedeutet ca. 8 bis 12 %, niederer Aschegehalt weniger als 4 % Asche. Der Schwefelgehalt der bevorzugt eingesetzten flotierten Kohle beträgt in der Regel weniger als 1 %.It goes without saying that coal with a high ash content is generally more difficult to disperse than coal with a low ash content. High ash content means approx. 8 to 12%, lower ash content less than 4% ash. The sulfur content of the preferably used floated coal is generally less than 1%.
Die Eigenschaften pumpbar und fließfähig betreffen die Viskosität der Kohledispersion. In der Regel ist eine Dispersion mit 2000 mPa.s gerade noch fließfähig. Für die Praxis, damit mit möglichst geringem Energieaufwand transportiert werden kann, liegen die gewünschten Werte bei 1000 mPa.s und darunter. Der optimal gewünschte Bereich kann mit kleiner 800 mPa.s angegeben werden. Er wird, wie in den Beispielen gezeigt, in den erfindungsgemäßen Kohledispersionen ohne weiteres erreicht.The pumpable and flowable properties relate to the viscosity of the coal dispersion. As a rule, a dispersion with 2000 mPa.s is just barely flowable. In practice, in order to be able to transport with as little energy as possible, the desired values are 1000 mPa.s and below. The optimally desired range can be specified with less than 800 mPa.s. As shown in the examples, it is easily achieved in the coal dispersions according to the invention.
Wie bereits erwähnt, können 1 bis 60 Gew.% des Wassers durch Methanol ersetzt werden. Der Zusatz von Methanol dient zum Zwecke der Viskositätserniedrigung (Pumpbarkeit) der Kohledispersionen bei Temperaturen unter 0°C (z. B. bis -20°C).As already mentioned, 1 to 60% by weight of the water can be replaced by methanol. The addition of methanol serves for the purpose of lowering the viscosity (pumpability) of the coal dispersions at temperatures below 0 ° C (e.g. to -20 ° C).
Darüberhinaus enthalten die erfindungsgemäßen Kohledispersionen die dem Fachmann an sich bekannten üblichen Zusätze:
- Schaumdämpfer, an sich übliche Schaumdämpfer wie Fettsäurepolyalkoxylate, z. B. Stearylalkoholpropoxylat mit 10 bis 50 Propylenoxideinheiten oder Silikonöle, etc.; als Viskositätsregler lösliche anorganische Salze, z. B. Ammoniumchlorid und -carbonat, sowie Alkali- und Erdalkalichloride und -carbonate, insbesondere des Natriums, Calciums und Magnesiums, wasserlösliche Phosphate und Silicate, wie Natrium-hexametaphosphat oder Natriummetasilikat-9-hydrat; pH-Wert-Regulatoren, da für die praktische Anwendung ein pH-Wert von 8 bis 10 besonders zweckmäßig ist, wie Alkali- und Erdalkalihydroxide, Ammoniak sowie primäre und sekundäre Amine; Stabilisierhilfsmittel mit Schutzkolloid- und/oder Verdickerwirkung, hierfür kommen in Betracht Polyether (z. B. Polyethylenoxid, Copolymere von Polyethylenoxid und Polypropylenoxid), Carboxymethylcellulose, Hydroxyethylcellulose, Polysaccharide (z. B. Alginate), Polyalkohole, Polyacrylate und Copolymere davon; als übliche Zusätze seien auch Biocide genannt.
- Foam damper, conventional foam damper such as fatty acid polyalkoxylates, e.g. B. stearyl alcohol propoxylate with 10 to 50 propylene oxide units or silicone oils, etc .; as a viscosity regulator soluble inorganic salts, e.g. B. ammonium chloride and carbonate, and alkali and alkaline earth metal chlorides and carbonates, especially sodium, Calcium and magnesium, water-soluble phosphates and silicates such as sodium hexametaphosphate or sodium metasilicate 9-hydrate; pH regulators, since a pH value of 8 to 10 is particularly expedient for practical use, such as alkali and alkaline earth metal hydroxides, ammonia and primary and secondary amines; Stabilizing aids with protective colloid and / or thickening action; polyethers (e.g. polyethylene oxide, copolymers of polyethylene oxide and polypropylene oxide), carboxymethyl cellulose, hydroxyethyl cellulose, polysaccharides (e.g. alginates), polyalcohols, polyacrylates and copolymers thereof are suitable for this; Biocides may also be mentioned as conventional additives.
Die Herstellung der erfindungsgemäß zu verwendenden Dispergiermittel ist an sich bekannt und erfolgt nach beschriebenen Verfahren. Der Grad der Ethoxylierung wird auf das mittlere Molekulargewicht, das sich aus der Hydroxylzahl des Gemisches ergibt, bezogen.The preparation of the dispersants to be used according to the invention is known per se and is carried out by the processes described. The degree of ethoxylation is based on the average molecular weight which results from the hydroxyl number of the mixture.
Die Herstellung der erfindungsgemäßen wäßrigen Kohledispersionen erfolgt in üblicher Weise. In der Regel wird eine konzentrierte wäßrige Lösung, die 40 bis 70 Gew.% erfindungsgemäßes Dispergiermittel enthält und die sich im Gegensatz zu manchen Dispergiermitteln des Standes der Technik leicht herstellen läßt, der Wassermenge zugegeben, der unter starkem Rühren die gemahlene Kohle und gegebenenfalls weitere Zusätze zugeführt werden.The aqueous coal dispersions according to the invention are prepared in a conventional manner. As a rule, a concentrated aqueous solution which contains 40 to 70% by weight of the dispersant according to the invention and which, in contrast to some dispersants of the prior art, can be easily prepared, is added to the amount of water which, with vigorous stirring, the ground coal and optionally further additives are fed.
A. Herstellung der erfindungsgemäßen Dispergiermittel Das Alkoholgemisch wird mit 1 Gew.% Kaliumhydroxid versetzt und unter Rühren bei 120 - 130°C portionsweise mit Ethylenoxid umgesetzt, wobei der Druck 10 bar nicht übersteigt. Das zu ethoxylierende Ausgangsmaterial hat folgende Zusammensetzung:
Die Viskosität der Dispersion [mPas] wird mit einem Rotationsviskosimeter bestimmt bei 20°C und einer Schergeschwindigkeit D von 220 s- .
Claims (3)
Applications Claiming Priority (2)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
DE3435945 | 1984-09-29 | ||
DE19843435945 DE3435945A1 (en) | 1984-09-29 | 1984-09-29 | AQUEOUS COAL DISPERSIONS |
Publications (3)
Publication Number | Publication Date |
---|---|
EP0176920A2 EP0176920A2 (en) | 1986-04-09 |
EP0176920A3 EP0176920A3 (en) | 1988-04-20 |
EP0176920B1 true EP0176920B1 (en) | 1990-02-07 |
Family
ID=6246790
Family Applications (1)
Application Number | Title | Priority Date | Filing Date |
---|---|---|---|
EP85112061A Expired - Lifetime EP0176920B1 (en) | 1984-09-29 | 1985-09-24 | Aqueous coal dispersions |
Country Status (7)
Country | Link |
---|---|
US (1) | US4657560A (en) |
EP (1) | EP0176920B1 (en) |
JP (1) | JPS6189295A (en) |
AU (1) | AU570900B2 (en) |
CA (1) | CA1261153A (en) |
DE (2) | DE3435945A1 (en) |
ZA (1) | ZA857521B (en) |
Families Citing this family (3)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
IT1184665B (en) * | 1985-10-24 | 1987-10-28 | Centro Speriment Metallurg | CHARCOAL-TAR MIX WITH HIGH SOLID CONTENT |
DE3621319A1 (en) * | 1986-06-26 | 1988-01-14 | Bayer Ag | Coal/water slurries having improved behaviour under shear stress |
RU2731605C1 (en) * | 2020-02-06 | 2020-09-04 | федеральное государственное автономное образовательное учреждение высшего образования «Национальный исследовательский Томский политехнический университет» | Fuel suspension |
Family Cites Families (15)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
GB1227345A (en) * | 1967-10-19 | 1971-04-07 | ||
US4242098A (en) * | 1978-07-03 | 1980-12-30 | Union Carbide Corporation | Transport of aqueous coal slurries |
JPS5620090A (en) * | 1979-07-26 | 1981-02-25 | Kao Corp | Dispersant for slurry of coal powder in water |
EP0043963A1 (en) * | 1980-06-30 | 1982-01-20 | Union Carbide Corporation | Improved process for ethoxylation of broad-range primary alcohols |
US4358293A (en) * | 1981-01-29 | 1982-11-09 | Gulf & Western Manufacturing Co. | Coal-aqueous mixtures |
SE443282B (en) * | 1981-06-25 | 1986-02-24 | Alfa Laval Ab | FAT PRODUCT FRIENDLY AT REFRIGERATOR TEMPERATURE AND PROCEDURE FOR PRODUCING THEREOF |
CA1180555A (en) * | 1981-09-14 | 1985-01-08 | Dai-Ichi Kogyo Seiyaku Co., Ltd. | High consistency-aqueous slurry of powdered coal |
JPS5845729A (en) * | 1981-09-14 | 1983-03-17 | Sanyo Chem Ind Ltd | Dispersant for high concn. coal-water slurry |
JPS5849794A (en) * | 1981-09-19 | 1983-03-24 | Sanyo Chem Ind Ltd | Dispersant for highly concentrated coal-water slurry |
JPS5896690A (en) * | 1981-12-03 | 1983-06-08 | Electric Power Dev Co Ltd | Preparation of concentrated coal slurry |
JPS58176294A (en) * | 1982-04-09 | 1983-10-15 | Chiyoda Chem Eng & Constr Co Ltd | Fine coal powder/alcohol composition and preparation thereof |
SE8202878L (en) * | 1982-05-07 | 1983-11-08 | Carbogel Ab | PUMPABLE WATER SLOPE OF A SOLID FUEL AND WAY TO PREPARE |
SE8202879L (en) * | 1982-05-07 | 1983-11-08 | Carbogel Ab | WATER SLUSHING OF A SOLID FUEL AND KITCHEN AND MEANS OF PREPARING THEREOF |
JPS5938288A (en) * | 1982-08-30 | 1984-03-02 | Kao Corp | Dispersion stabilizer for aqueous coal powder slurry |
JPS5943095A (en) * | 1982-09-06 | 1984-03-09 | Mitsui Toatsu Chem Inc | Liquid/solid suspension fuel |
-
1984
- 1984-09-29 DE DE19843435945 patent/DE3435945A1/en not_active Withdrawn
-
1985
- 1985-09-24 EP EP85112061A patent/EP0176920B1/en not_active Expired - Lifetime
- 1985-09-24 DE DE8585112061T patent/DE3575944D1/en not_active Expired - Lifetime
- 1985-09-27 JP JP60212756A patent/JPS6189295A/en active Pending
- 1985-09-30 ZA ZA857521A patent/ZA857521B/en unknown
- 1985-09-30 CA CA000491854A patent/CA1261153A/en not_active Expired
- 1985-09-30 US US06/781,888 patent/US4657560A/en not_active Expired - Fee Related
- 1985-10-01 AU AU48277/85A patent/AU570900B2/en not_active Ceased
Also Published As
Publication number | Publication date |
---|---|
EP0176920A2 (en) | 1986-04-09 |
JPS6189295A (en) | 1986-05-07 |
AU4827785A (en) | 1986-05-08 |
US4657560A (en) | 1987-04-14 |
EP0176920A3 (en) | 1988-04-20 |
DE3435945A1 (en) | 1986-04-03 |
CA1261153A (en) | 1989-09-26 |
AU570900B2 (en) | 1988-03-24 |
DE3575944D1 (en) | 1990-03-15 |
ZA857521B (en) | 1986-06-25 |
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