EP0660964B2 - Werkstoff für elektrische kontakte auf der basis von silber-zinnoxid oder silber-zinkoxid und verfahren zu seiner herstellung - Google Patents
Werkstoff für elektrische kontakte auf der basis von silber-zinnoxid oder silber-zinkoxid und verfahren zu seiner herstellung Download PDFInfo
- Publication number
- EP0660964B2 EP0660964B2 EP93920746A EP93920746A EP0660964B2 EP 0660964 B2 EP0660964 B2 EP 0660964B2 EP 93920746 A EP93920746 A EP 93920746A EP 93920746 A EP93920746 A EP 93920746A EP 0660964 B2 EP0660964 B2 EP 0660964B2
- Authority
- EP
- European Patent Office
- Prior art keywords
- tin oxide
- silver
- powder
- mixture
- weight
- 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
Links
Classifications
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01H—ELECTRIC SWITCHES; RELAYS; SELECTORS; EMERGENCY PROTECTIVE DEVICES
- H01H1/00—Contacts
- H01H1/02—Contacts characterised by the material thereof
- H01H1/021—Composite material
- H01H1/023—Composite material having a noble metal as the basic material
- H01H1/0237—Composite material having a noble metal as the basic material and containing oxides
- H01H1/02372—Composite material having a noble metal as the basic material and containing oxides containing as major components one or more oxides of the following elements only: Cd, Sn, Zn, In, Bi, Sb or Te
-
- C—CHEMISTRY; METALLURGY
- C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
- C22C—ALLOYS
- C22C1/00—Making non-ferrous alloys
- C22C1/04—Making non-ferrous alloys by powder metallurgy
- C22C1/05—Mixtures of metal powder with non-metallic powder
- C22C1/059—Making alloys comprising less than 5% by weight of dispersed reinforcing phases
-
- C—CHEMISTRY; METALLURGY
- C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
- C22C—ALLOYS
- C22C32/00—Non-ferrous alloys containing at least 5% by weight but less than 50% by weight of oxides, carbides, borides, nitrides, silicides or other metal compounds, e.g. oxynitrides, sulfides, whether added as such or formed in situ
- C22C32/001—Non-ferrous alloys containing at least 5% by weight but less than 50% by weight of oxides, carbides, borides, nitrides, silicides or other metal compounds, e.g. oxynitrides, sulfides, whether added as such or formed in situ with only oxides
- C22C32/0015—Non-ferrous alloys containing at least 5% by weight but less than 50% by weight of oxides, carbides, borides, nitrides, silicides or other metal compounds, e.g. oxynitrides, sulfides, whether added as such or formed in situ with only oxides with only single oxides as main non-metallic constituents
- C22C32/0021—Matrix based on noble metals, Cu or alloys thereof
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01H—ELECTRIC SWITCHES; RELAYS; SELECTORS; EMERGENCY PROTECTIVE DEVICES
- H01H1/00—Contacts
- H01H1/02—Contacts characterised by the material thereof
- H01H1/021—Composite material
- H01H1/023—Composite material having a noble metal as the basic material
- H01H1/0237—Composite material having a noble metal as the basic material and containing oxides
- H01H1/02372—Composite material having a noble metal as the basic material and containing oxides containing as major components one or more oxides of the following elements only: Cd, Sn, Zn, In, Bi, Sb or Te
- H01H1/02376—Composite material having a noble metal as the basic material and containing oxides containing as major components one or more oxides of the following elements only: Cd, Sn, Zn, In, Bi, Sb or Te containing as major component SnO2
-
- 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
- Y10T—TECHNICAL SUBJECTS COVERED BY FORMER US CLASSIFICATION
- Y10T428/00—Stock material or miscellaneous articles
- Y10T428/12—All metal or with adjacent metals
- Y10T428/12014—All metal or with adjacent metals having metal particles
- Y10T428/12028—Composite; i.e., plural, adjacent, spatially distinct metal components [e.g., layers, etc.]
- Y10T428/12049—Nonmetal component
- Y10T428/12056—Entirely inorganic
-
- 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
- Y10T—TECHNICAL SUBJECTS COVERED BY FORMER US CLASSIFICATION
- Y10T428/00—Stock material or miscellaneous articles
- Y10T428/12—All metal or with adjacent metals
- Y10T428/12014—All metal or with adjacent metals having metal particles
- Y10T428/12028—Composite; i.e., plural, adjacent, spatially distinct metal components [e.g., layers, etc.]
- Y10T428/12063—Nonparticulate metal component
- Y10T428/12097—Nonparticulate component encloses particles
-
- 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
- Y10T—TECHNICAL SUBJECTS COVERED BY FORMER US CLASSIFICATION
- Y10T428/00—Stock material or miscellaneous articles
- Y10T428/12—All metal or with adjacent metals
- Y10T428/12014—All metal or with adjacent metals having metal particles
- Y10T428/12028—Composite; i.e., plural, adjacent, spatially distinct metal components [e.g., layers, etc.]
- Y10T428/12063—Nonparticulate metal component
- Y10T428/12104—Particles discontinuous
-
- 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
- Y10T—TECHNICAL SUBJECTS COVERED BY FORMER US CLASSIFICATION
- Y10T428/00—Stock material or miscellaneous articles
- Y10T428/12—All metal or with adjacent metals
- Y10T428/12014—All metal or with adjacent metals having metal particles
- Y10T428/12028—Composite; i.e., plural, adjacent, spatially distinct metal components [e.g., layers, etc.]
- Y10T428/12146—Nonmetal particles in a component
Definitions
- the invention is based on a material for electrical contacts based on silver-tin oxide with those specified in the preamble of claim 1 Features.
- a material is from WO 80/01434 known; the material is obtained by mixing a powder of silver or one mainly Silver containing alloy with tin oxide powder, compacting of mixing and sintering.
- Bismuth and germanium oxide are also additives have been mentioned (DE-A-31 02 067 and DE-A-32 32 627). These additives help to wet tin oxide particles, so that if the contact piece surface under the Effect of a switching arc melts locally, the Tin oxide remains in fine suspension. Besides this positive effect in terms of heating behavior under continuous current, however, these additives have also undesirable side effects.
- Another disadvantage in particular of tungsten and molybdenum compounds in that they are particularly in switching mode AC1 load (DIN 57660 part 102) a material transfer favor the accelerated burnup and thus leads to a reduction in the service life.
- a contact material with little tendency to weld and if possible low contact temperature under continuous current load be obtained by targeting one Fabricates in which areas where no or contains very little metal oxide with areas where all or the far predominant part of the metal oxide component in fine Distribution is included.
- a composite powder which the predominant Part of the tin oxide and other oxides and / or carbides and part of the silver.
- This composite powder is mixed with the rest of the silver powder and possibly with the smaller rest of the metal oxides mixed, compacted, sintered and formed. To this Way you get a usable material, however, after a relatively complex Method.
- the oxides of tungsten are as metal oxides, Molybdenum, bismuth, vanadium and copper called.
- the doped tin oxide powder is one Composite powder, which can be obtained by Mix the tin oxide powder with the powder Dopant, annealing the mixture so that the Dopant and the tin oxide powder particles diffuse, and separating the excess dopant of tin oxide powder.
- To obtain doped tin oxide powder is in P 42 19 333.8 discloses a solution of a salt of tin and a salt of the metal or metals from which Oxides or carbides are the dopant in a hot, oxidizing atmosphere spray in which the salts are decomposed so that a fine-particle composite powder precipitates, its particles contains the tin oxide and the dopants.
- the present invention is based on the object a material of the type mentioned at the beginning create the addition of an equally favorable heating behavior shows how the known contact materials, however, is more ductile and one in the AC1 switching case has a longer lifespan.
- This task is solved by a material with the specified in claim 1 Features.
- a particularly suitable process for the manufacture of such a material is the subject of claim 8.
- Advantageous further developments the invention are the subject of the dependent claims.
- the invention additionally uses a powder which contains one or more chemical compounds of silver, oxygen and a metal from subgroups II to VI and / or antimony, bismuth, germanium, gallium and indium, in particular silver-tungsten-oxygen compounds, silver-molybdenum-oxygen compounds, silver-antimony-oxygen compounds, silver-bismuth-oxygen compounds and silver-germanium-oxygen compounds.
- this class of compounds also includes silver antimonate and silver molybdate, of which Christine Bourda (see above) is known to be in a silver-tin oxide-molybdenum oxide material or silver-tin oxide-antimony oxide material.
- Another advantage of the invention is that due to the lower proportion of the chosen additive the service life of contact pieces made of the material is increased, especially under AC1-test conditions.
- the use of the invention Powder surprisingly leads to one less erosion than with conventional silver-tin oxide contact materials with pure metal oxide additives such as tungsten oxide, molybdenum oxide or bismuth oxide.
- the tin oxide particles are superficially with the silver-metal-oxygen compounds busy. They promote the wetting of the tin oxide particles with the arc forming melt phase then particularly effective.
- a tin oxide powder modified in this way can be obtained with advantage by using tin oxide powder and the powdery additive together mixed and glows together so that the tin oxide powder particles be wetted by the additive, whereby a Part of the addition also in the surface area of the Diffuse tin oxide particles and possibly a mixed oxide can form.
- the material expediently contains 5 to 20% by weight, preferably 8 to 14 %
- the tin oxide powder preferably with at least 0.1% by weight of the additive, but with no more than 2.5% by weight, preferably with not more than 1% by weight of the additive.
- Silver molybdate is particularly preferred as an additive because of its particularly beneficial effect on the Heating behavior.
- the glow of the mixture of tin oxide and the selected addition is conveniently made at oxygen-containing atmosphere, preferably in air at a Temperature between 500 ° C and 800 ° C, best at a temperature just above the melting point of the additive so that it becomes liquid and the tin oxide particles are wetted superficially.
- the addition is then only there where its wetting Effect is desired, and can therefore be economical be used. With the small amounts, in the tin oxide particles stick to not yet with each other; but should it be in individual cases can occur by grinding to encounter.
- the tin oxide and the additive can not only connected by glowing together but also by separating the additive on the tin oxide particles using chemical or physical deposition processes.
- the teaching according to the invention can be transferred are based on contact materials based on silver with zinc oxide. In such materials are so far in in practice, no additives are used, but one endeavors to take constructive measures in the shaft device to achieve a reduction in the contact point temperature.
- an additive combined zinc oxide powder can a lowering of the contact point temperature also with this type of material to reach.
- the three examples can be modified accordingly that zinc oxide is used instead of tin oxide becomes.
Landscapes
- Chemical & Material Sciences (AREA)
- Engineering & Computer Science (AREA)
- Materials Engineering (AREA)
- Mechanical Engineering (AREA)
- Metallurgy (AREA)
- Organic Chemistry (AREA)
- Composite Materials (AREA)
- Dispersion Chemistry (AREA)
- Contacts (AREA)
- Powder Metallurgy (AREA)
- Manufacture Of Alloys Or Alloy Compounds (AREA)
- Conductive Materials (AREA)
Description
Claims (13)
- Werkstoff für elektrische Kontakte auf der Basis von Silber-Zinnoxid, der erhalten wird durchMischen eines Pulvers aus Silber oder aus einer hauptsächlich Silber enthaltenden Legierung mit Zinnoxidpulver,Verdichten der Mischung undSintern,
- Werkstoff nach Anspruch 1, dadurch gekennzeichnet, daß er 5 bis 20 Gew.-% Zinnoxid enthält.
- Werkstoff nach Anspruch 2, dadurch gekennzeichnet, daß er 8 bis 14 Gew.-% Zinnoxid enthält.
- Werkstoff nach einem der vorstehenden Ansprüche dadurch gekennzeichnet, daß der Zusatz in einer Menge von mindestens 0,1 Gew.-% vorhanden ist.
- Werkstoff nach einem der vorstehenden Ansprüche, dadurch gekennzeichnet, dass der Zusatz in einer Menge von nicht mehr als 2,5 Gew.-% vorhanden ist.
- Werkstoff nach Anspruch 5, dadurch gekennzeichnet, dass der Zusatz in einer Menge von nicht mehr als 1 Gew.-% vorhanden ist.
- Werkstoff nach einem der vorstehenden Ansprüche, dadurch gekennzeichnet, dass die im Zusatz enthaltenen Verbindungen ein Metall aus der Gruppe Wolfram, Molybdän, Vanadium, Antimon, Wismut und Germanium enthalten, wobei Molybdän besonders bevorzugt ist.
- Verfahren zum Herstellen eines Werkstoffs für elektrische Kontakte auf der Basis von Silber-Zinnoxid durch Mischen eines Pulvers aus Silber oder aus einer hauptsächlich Silber enthaltenden Legierung mit Zinnoxidpulver und einem zusätzlichen Pulver, welches 0,01 bis 10 Gew.-% bezogen auf die Menge des Zinnoxids einer oder mehrerer Verbindungen enthält, die aus Silber, Sauerstoff und einem Metall aus den Nebengruppen II bis VI des PERIODISCHEN SYSTEMS und/oder Antimon, Wismut, Germanium, Indium und Gallium bestehen, Verdichten der Mischung und Sintern gemäß einem der vorstehenden Ansprüche, dadurch gekennzeichnet, daß das hauptsächlich aus Zinnoxid und dem Zusatz bestehende Pulver erhalten wird, durchMischen des Zinnoxidpulvers mit dem Zusatz in Pulverform undGlühen der Mischung.
- Verfahren nach Anspruch 8, dadurch gekennzeichnet, daß die Mischung an Luft geglüht wird.
- Verfahren nach Ansrpuch 8 oder 9, dadurch gekennzeichnet, daß die Mischung zwischen 500° C und 800°C geglüht wird.
- Verfahren nach einem der Ansprüche 8 bis 10, dadurch gekennzeichnet, daß die Mischung bei einer oberhalb des Schmelzpunktes des Zusatzes liegenden Temperatur geglüht wird.
- Verfahren nach einem der Ansprüche 8 bis 11, dadurch gekennzeichnet, daß der Werkstoff nach dem Sintern nachverdichtet und/oder umgeformt wird.
- Werkstoff nach einem der Ansprüche 1 bis 7 oder hergestellt nach einem der Anspüche 8 bis 12, dadurch gekennzeichnet, daß das Zinnoxid durch Zinkoxid ersetzt ist.
Applications Claiming Priority (3)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
DE4231022 | 1992-09-16 | ||
DE4231022 | 1992-09-16 | ||
PCT/EP1993/002511 WO1994007252A1 (de) | 1992-09-16 | 1993-09-16 | Werkstoff für elektrische kontakte auf der basis von silber-zinnoxid oder silber-zinkoxid und verfahren zu seiner herstellung |
Publications (3)
Publication Number | Publication Date |
---|---|
EP0660964A1 EP0660964A1 (de) | 1995-07-05 |
EP0660964B1 EP0660964B1 (de) | 1996-06-26 |
EP0660964B2 true EP0660964B2 (de) | 2003-01-08 |
Family
ID=6468120
Family Applications (1)
Application Number | Title | Priority Date | Filing Date |
---|---|---|---|
EP93920746A Expired - Lifetime EP0660964B2 (de) | 1992-09-16 | 1993-09-16 | Werkstoff für elektrische kontakte auf der basis von silber-zinnoxid oder silber-zinkoxid und verfahren zu seiner herstellung |
Country Status (7)
Country | Link |
---|---|
US (1) | US5822674A (de) |
EP (1) | EP0660964B2 (de) |
JP (1) | JP3441074B2 (de) |
AT (1) | ATE139864T1 (de) |
DE (2) | DE59303090D1 (de) |
ES (1) | ES2091633T5 (de) |
WO (1) | WO1994007252A1 (de) |
Families Citing this family (8)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
DE19503182C1 (de) * | 1995-02-01 | 1996-05-15 | Degussa | Sinterwerkstoff auf der Basis Silber-Zinnoxid für elektrische Kontakte und Verfahren zu dessen Herstellung |
US5846288A (en) * | 1995-11-27 | 1998-12-08 | Chemet Corporation | Electrically conductive material and method for making |
EP2644723B1 (de) | 2012-03-26 | 2017-01-18 | Umicore AG & Co. KG | Verbundwerkstoff |
CN104493175B (zh) * | 2014-12-30 | 2016-04-13 | 桂林电器科学研究院有限公司 | 一种含添加物的银氧化锡电触头材料的制备方法 |
RU2579846C1 (ru) * | 2015-03-11 | 2016-04-10 | Федеральное государственное автономное образовательное учреждение высшего образования "Сибирский федеральный университет" | Способ получения легированного оксидом висмута серебряно-оловооксидного материала для электроконтактов |
DE102016105437A1 (de) | 2016-03-23 | 2017-09-28 | Doduco Gmbh | Verfahren zur Herstellung eines Kontaktwerkstoffes auf Basis von Silber-Zinnoxid oder Silber-Sinkoxid sowie Kontaktwerkstoff |
US10290434B2 (en) | 2016-09-23 | 2019-05-14 | Honeywell International Inc. | Silver metal oxide alloy and method of making |
CN115870498A (zh) * | 2022-12-06 | 2023-03-31 | 浙江福达合金材料科技有限公司 | 一种提高片状银氧化锡电触头材料结合强度的制备方法 |
Family Cites Families (19)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
US3685134A (en) * | 1970-05-15 | 1972-08-22 | Mallory & Co Inc P R | Method of making electrical contact materials |
CH588152A5 (de) * | 1972-12-11 | 1977-05-31 | Siemens Ag | |
US4141727A (en) * | 1976-12-03 | 1979-02-27 | Matsushita Electric Industrial Co., Ltd. | Electrical contact material and method of making the same |
DE2659012C3 (de) * | 1976-12-27 | 1980-01-24 | Siemens Ag, 1000 Berlin Und 8000 Muenchen | Verfahren zum Herstellen eines Sinterkontaktwerkstoffes aus Silber und eingelagerten Metalloxiden |
US4294616A (en) * | 1979-01-02 | 1981-10-13 | Gte Products Corporation | Electrical contacts |
DE2933338C3 (de) * | 1979-08-17 | 1983-04-28 | Degussa Ag, 6000 Frankfurt | Werkstoff für elektrische Kontakte und Verfahren zu seiner Herstellung |
DE2952128C2 (de) * | 1979-12-22 | 1984-10-11 | Degussa Ag, 6000 Frankfurt | Verfahren zur Vorbehandlung des Pulvers für gesintertes und stranggepreßtes Halbzeug aus Silber-Zinnoxid für elektrische Kontakte |
DE3017424A1 (de) * | 1980-05-07 | 1981-11-12 | Degussa Ag, 6000 Frankfurt | Werkstoff fuer elektrische kontakte |
DE3102067A1 (de) * | 1981-01-23 | 1982-08-19 | Degussa Ag, 6000 Frankfurt | Werkstoff fuer elektrische kontakte |
DE3232627A1 (de) * | 1981-09-24 | 1983-04-07 | Doduco KG Dr. Eugen Dürrwächter, 7530 Pforzheim | Werkstoff fuer elektrische kontakte |
DE3146972A1 (de) * | 1981-11-26 | 1983-06-01 | Siemens AG, 1000 Berlin und 8000 München | Verfahren zum herstellen von formteilen aus cadmiumfreien silber-metalloxid-verbundwerkstoffen fuer elektrische kontaktstuecke |
DE3305270A1 (de) * | 1983-02-16 | 1984-08-16 | Siemens AG, 1000 Berlin und 8000 München | Sinterverbundwerkstoff fuer elektrische kontakte und verfahren zu seiner herstellung |
DE3402091C2 (de) * | 1984-01-21 | 1994-01-13 | Rau Gmbh G | Verbundwerkstoff für elektrische Kontaktstücke |
DE3421758A1 (de) * | 1984-06-12 | 1985-12-12 | Siemens AG, 1000 Berlin und 8000 München | Sinterkontaktwerkstoff fuer niederspannungsschaltgeraete der energietechnik und verfahren zu dessen herstellung |
DE3426240A1 (de) * | 1984-07-17 | 1986-01-30 | Doduco KG Dr. Eugen Dürrwächter, 7530 Pforzheim | Verfahren zum herstellen eines bandfoermigen halbzeugs fuer elektrische kontakte aus einem verbundmaterial und vorrichtung zum durchfuehren des verfahrens |
WO1989009478A1 (en) * | 1988-03-26 | 1989-10-05 | Doduco Gmbh + Co. Dr. Eugen Dürrwächter | Semifinished product for electrical contacts, made of a composite material based on silver and tin oxide, and powder metallurgical process for producing it |
EP0369283B1 (de) * | 1988-11-17 | 1994-09-14 | Siemens Aktiengesellschaft | Sinterkontaktwerkstoff für Niederspannungsschaltgeräte der Energietechnik, insbesondere für Motorschütze |
DE69032065T2 (de) * | 1989-12-26 | 1998-10-29 | Sumitomo Metal Mining Co | Verbundwerkstoff von Silber und Metalloxyd und Verfahren zur Herstellung desselben |
DE4319137A1 (de) * | 1992-06-10 | 1993-12-16 | Duerrwaechter E Dr Doduco | Werkstoff für elektrische Kontakte auf der Basis von Silber-Zinnoxid oder Siler-Zinkoxid |
-
1993
- 1993-09-16 AT AT93920746T patent/ATE139864T1/de not_active IP Right Cessation
- 1993-09-16 DE DE59303090T patent/DE59303090D1/de not_active Expired - Lifetime
- 1993-09-16 DE DE4331526A patent/DE4331526C3/de not_active Expired - Fee Related
- 1993-09-16 ES ES93920746T patent/ES2091633T5/es not_active Expired - Lifetime
- 1993-09-16 EP EP93920746A patent/EP0660964B2/de not_active Expired - Lifetime
- 1993-09-16 US US08/397,149 patent/US5822674A/en not_active Expired - Lifetime
- 1993-09-16 JP JP50779894A patent/JP3441074B2/ja not_active Expired - Fee Related
- 1993-09-16 WO PCT/EP1993/002511 patent/WO1994007252A1/de active IP Right Grant
Also Published As
Publication number | Publication date |
---|---|
DE59303090D1 (de) | 1996-08-01 |
US5822674A (en) | 1998-10-13 |
ES2091633T5 (es) | 2003-09-01 |
DE4331526C2 (de) | 1998-07-30 |
EP0660964A1 (de) | 1995-07-05 |
ES2091633T3 (es) | 1996-11-01 |
JPH08504292A (ja) | 1996-05-07 |
EP0660964B1 (de) | 1996-06-26 |
JP3441074B2 (ja) | 2003-08-25 |
DE4331526C3 (de) | 2003-11-06 |
DE4331526A1 (de) | 1994-03-17 |
ATE139864T1 (de) | 1996-07-15 |
WO1994007252A1 (de) | 1994-03-31 |
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