JPH09505511A - 触媒前駆体組成物、及びその製造方法 - Google Patents
触媒前駆体組成物、及びその製造方法Info
- Publication number
- JPH09505511A JPH09505511A JP7508748A JP50874895A JPH09505511A JP H09505511 A JPH09505511 A JP H09505511A JP 7508748 A JP7508748 A JP 7508748A JP 50874895 A JP50874895 A JP 50874895A JP H09505511 A JPH09505511 A JP H09505511A
- Authority
- JP
- Japan
- Prior art keywords
- metallocene
- catalyst
- composition
- group
- cationic
- 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.)
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J31/00—Catalysts comprising hydrides, coordination complexes or organic compounds
- B01J31/02—Catalysts comprising hydrides, coordination complexes or organic compounds containing organic compounds or metal hydrides
- B01J31/12—Catalysts comprising hydrides, coordination complexes or organic compounds containing organic compounds or metal hydrides containing organo-metallic compounds or metal hydrides
- B01J31/14—Catalysts comprising hydrides, coordination complexes or organic compounds containing organic compounds or metal hydrides containing organo-metallic compounds or metal hydrides of aluminium or boron
- B01J31/143—Catalysts comprising hydrides, coordination complexes or organic compounds containing organic compounds or metal hydrides containing organo-metallic compounds or metal hydrides of aluminium or boron of aluminium
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J31/00—Catalysts comprising hydrides, coordination complexes or organic compounds
- B01J31/02—Catalysts comprising hydrides, coordination complexes or organic compounds containing organic compounds or metal hydrides
- B01J31/06—Catalysts comprising hydrides, coordination complexes or organic compounds containing organic compounds or metal hydrides containing polymers
- B01J31/08—Ion-exchange resins
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J31/00—Catalysts comprising hydrides, coordination complexes or organic compounds
- B01J31/02—Catalysts comprising hydrides, coordination complexes or organic compounds containing organic compounds or metal hydrides
- B01J31/06—Catalysts comprising hydrides, coordination complexes or organic compounds containing organic compounds or metal hydrides containing polymers
- B01J31/08—Ion-exchange resins
- B01J31/10—Ion-exchange resins sulfonated
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J31/00—Catalysts comprising hydrides, coordination complexes or organic compounds
- B01J31/02—Catalysts comprising hydrides, coordination complexes or organic compounds containing organic compounds or metal hydrides
- B01J31/12—Catalysts comprising hydrides, coordination complexes or organic compounds containing organic compounds or metal hydrides containing organo-metallic compounds or metal hydrides
- B01J31/14—Catalysts comprising hydrides, coordination complexes or organic compounds containing organic compounds or metal hydrides containing organo-metallic compounds or metal hydrides of aluminium or boron
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J31/00—Catalysts comprising hydrides, coordination complexes or organic compounds
- B01J31/16—Catalysts comprising hydrides, coordination complexes or organic compounds containing coordination complexes
- B01J31/165—Polymer immobilised coordination complexes, e.g. organometallic complexes
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J31/00—Catalysts comprising hydrides, coordination complexes or organic compounds
- B01J31/16—Catalysts comprising hydrides, coordination complexes or organic compounds containing coordination complexes
- B01J31/22—Organic complexes
- B01J31/2282—Unsaturated compounds used as ligands
- B01J31/2295—Cyclic compounds, e.g. cyclopentadienyls
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- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08F—MACROMOLECULAR COMPOUNDS OBTAINED BY REACTIONS ONLY INVOLVING CARBON-TO-CARBON UNSATURATED BONDS
- C08F10/00—Homopolymers and copolymers of unsaturated aliphatic hydrocarbons having only one carbon-to-carbon double bond
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J2531/00—Additional information regarding catalytic systems classified in B01J31/00
- B01J2531/40—Complexes comprising metals of Group IV (IVA or IVB) as the central metal
- B01J2531/48—Zirconium
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J2531/00—Additional information regarding catalytic systems classified in B01J31/00
- B01J2531/40—Complexes comprising metals of Group IV (IVA or IVB) as the central metal
- B01J2531/49—Hafnium
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- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08F—MACROMOLECULAR COMPOUNDS OBTAINED BY REACTIONS ONLY INVOLVING CARBON-TO-CARBON UNSATURATED BONDS
- C08F4/00—Polymerisation catalysts
- C08F4/42—Metals; Metal hydrides; Metallo-organic compounds; Use thereof as catalyst precursors
- C08F4/44—Metals; Metal hydrides; Metallo-organic compounds; Use thereof as catalyst precursors selected from light metals, zinc, cadmium, mercury, copper, silver, gold, boron, gallium, indium, thallium, rare earths or actinides
- C08F4/60—Metals; Metal hydrides; Metallo-organic compounds; Use thereof as catalyst precursors selected from light metals, zinc, cadmium, mercury, copper, silver, gold, boron, gallium, indium, thallium, rare earths or actinides together with refractory metals, iron group metals, platinum group metals, manganese, rhenium technetium or compounds thereof
- C08F4/619—Component covered by group C08F4/60 containing a transition metal-carbon bond
- C08F4/61908—Component covered by group C08F4/60 containing a transition metal-carbon bond in combination with an ionising compound other than alumoxane, e.g. (C6F5)4B-X+
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- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08F—MACROMOLECULAR COMPOUNDS OBTAINED BY REACTIONS ONLY INVOLVING CARBON-TO-CARBON UNSATURATED BONDS
- C08F4/00—Polymerisation catalysts
- C08F4/42—Metals; Metal hydrides; Metallo-organic compounds; Use thereof as catalyst precursors
- C08F4/44—Metals; Metal hydrides; Metallo-organic compounds; Use thereof as catalyst precursors selected from light metals, zinc, cadmium, mercury, copper, silver, gold, boron, gallium, indium, thallium, rare earths or actinides
- C08F4/60—Metals; Metal hydrides; Metallo-organic compounds; Use thereof as catalyst precursors selected from light metals, zinc, cadmium, mercury, copper, silver, gold, boron, gallium, indium, thallium, rare earths or actinides together with refractory metals, iron group metals, platinum group metals, manganese, rhenium technetium or compounds thereof
- C08F4/619—Component covered by group C08F4/60 containing a transition metal-carbon bond
- C08F4/61912—Component covered by group C08F4/60 containing a transition metal-carbon bond in combination with an organoaluminium compound
-
- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08F—MACROMOLECULAR COMPOUNDS OBTAINED BY REACTIONS ONLY INVOLVING CARBON-TO-CARBON UNSATURATED BONDS
- C08F4/00—Polymerisation catalysts
- C08F4/42—Metals; Metal hydrides; Metallo-organic compounds; Use thereof as catalyst precursors
- C08F4/44—Metals; Metal hydrides; Metallo-organic compounds; Use thereof as catalyst precursors selected from light metals, zinc, cadmium, mercury, copper, silver, gold, boron, gallium, indium, thallium, rare earths or actinides
- C08F4/60—Metals; Metal hydrides; Metallo-organic compounds; Use thereof as catalyst precursors selected from light metals, zinc, cadmium, mercury, copper, silver, gold, boron, gallium, indium, thallium, rare earths or actinides together with refractory metals, iron group metals, platinum group metals, manganese, rhenium technetium or compounds thereof
- C08F4/619—Component covered by group C08F4/60 containing a transition metal-carbon bond
- C08F4/61916—Component covered by group C08F4/60 containing a transition metal-carbon bond supported on a carrier, e.g. silica, MgCl2, polymer
-
- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08F—MACROMOLECULAR COMPOUNDS OBTAINED BY REACTIONS ONLY INVOLVING CARBON-TO-CARBON UNSATURATED BONDS
- C08F4/00—Polymerisation catalysts
- C08F4/42—Metals; Metal hydrides; Metallo-organic compounds; Use thereof as catalyst precursors
- C08F4/44—Metals; Metal hydrides; Metallo-organic compounds; Use thereof as catalyst precursors selected from light metals, zinc, cadmium, mercury, copper, silver, gold, boron, gallium, indium, thallium, rare earths or actinides
- C08F4/60—Metals; Metal hydrides; Metallo-organic compounds; Use thereof as catalyst precursors selected from light metals, zinc, cadmium, mercury, copper, silver, gold, boron, gallium, indium, thallium, rare earths or actinides together with refractory metals, iron group metals, platinum group metals, manganese, rhenium technetium or compounds thereof
- C08F4/619—Component covered by group C08F4/60 containing a transition metal-carbon bond
- C08F4/6192—Component covered by group C08F4/60 containing a transition metal-carbon bond containing at least one cyclopentadienyl ring, condensed or not, e.g. an indenyl or a fluorenyl ring
- C08F4/61922—Component covered by group C08F4/60 containing a transition metal-carbon bond containing at least one cyclopentadienyl ring, condensed or not, e.g. an indenyl or a fluorenyl ring containing at least two cyclopentadienyl rings, fused or not
-
- 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
- Y10S526/00—Synthetic resins or natural rubbers -- part of the class 520 series
- Y10S526/943—Polymerization with metallocene catalysts
Landscapes
- Chemical & Material Sciences (AREA)
- Organic Chemistry (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Engineering & Computer Science (AREA)
- Materials Engineering (AREA)
- Inorganic Chemistry (AREA)
- Health & Medical Sciences (AREA)
- Medicinal Chemistry (AREA)
- Polymers & Plastics (AREA)
- Crystallography & Structural Chemistry (AREA)
- Transition And Organic Metals Composition Catalysts For Addition Polymerization (AREA)
- Catalysts (AREA)
Abstract
Description
Claims (1)
- 【特許請求の範囲】 1.交換可能なカチオン性部位のうちの少なくともいくつかが触媒的カチオン 性メタロセン種からなるカチオン交換樹脂を含んでなる触媒前駆体組成物。 2.メタロセン種がCpmMAnBp(式中、Cpは非置換またはモノ−若しく はポリ−置換シクロペンタジエニル基であり、Mはメタロセン−形成金属原子で あり、そしてA及びBは同一であっても異なっていてもよいハロゲン原子、水素 原子、ヒドロキシル基、アルコキシド基若しくはアルキル基を表し、そしてmは 1若しくは2、m+n+pはMの原子価に等しい。)によって与えられる、請求 項1に記載の組成物。 3.メタロセン−形成金属原子がジルコニウムまたはハフニウムである、請求 項2に記載の組成物。 4.樹脂がスルホネート基からなるアニオン性部位を含む、請求項1に記載の 組成物。 5.CpmMAnBpがビス−(インデニル)ジルコニウムジハライドである、 請求項2に記載の組成物。 6.CpmMAnBpが組成物の0.01〜2.0ミリモル/gを構成する、請 求項2に記載の組成物。 7.CpmMAnBpが組成物の0.01〜1.0ミリモル/gを構成する、請 求項6に記載の組成物。 8.カチオン性交換部位がPh3C+で交換できる、請求項1に記載の組成物。 9.カチオン交換樹脂を強度にルイス酸性のカチオン性種と接触させて中間体 を形成すること;及び中間体をメタロセンと接触させて触媒的にカチオン性のメ タロセン種を形成することを含んで成る、請求項1記載の触媒前駆体組成物の製 造方法。 10.前記の強度にルイス酸性カチオン性種がPh3C+である、請求項9に記 載の方法。 11. 前記のPh3C+がトリチルハライドの形態で与えられる、請求項10 に記載の方法。 12.前記メタロセンがCpmMAnBp(式中、Cpは非置換またはモノ−若 しくはポリ−置換シクロペンタジエニル基であり、Mはメタロセン−形成金属原 子であり、そしてA及びBは同一であっても異なっていてもよいハロゲン原子、 水素原子、ヒドロキシル基、アルコキシド基若しくはアルキル基を表し、そして mは1若しくは2、m+n+pはMの原子価に等しい。)である、請求項9に記 載の方法。 13.請求項1記載の触媒前駆体組成物と組み合わされたアルキルアルミニウ ム化合物を含んで成る触媒。 14.アルキルアルミニウム化合物のアルキル基が1〜10個の炭素原子を含 む、請求項13に記載の触媒。 15.アルキルアルミニウム化合物がアルキルアルミニウムモノハライド、ア ルキルアルミニウムジハライド、及びトリアルキルアルミニウムより成る群から 選択される、請求項13に記載の触媒。 16.トリアルキルアルミニウムがトリメチルアルミニウム、トリエチルアル ミニウム及びトリイソブチルアルミニウムより成る群から選択される、請求項1 5に記載の触媒。 17.トリアルキルアルミニウムがトリイソブチルアルミニウムである、請求 項15に記載の触媒。 18.オレフィンポリマーの製造方法であって、相当するモノマーを請求項1 3記載の触媒と接触させることを含んで成る前記の方法。 19.オレフィンポリマーがエチレンのホモポリマー、またはエチレンと少な くとも1種のアルファ−オレフィンとのコポリマーである、請求項18に記載の 方法。 20.担持された触媒的にカチオン性のメタロセン種を、相当するメタロセン から製造するための、強度にルイス酸性のカチオン性メタロセン種での交換によ って変性されたカチオン交換樹脂の使用。 21.強度に酸性のカチオン性種がPh3C+である、請求項20に記載のカチ オン交換樹脂の使用。 22.相当するメタロセンはCpmMAnBp(式中、Cpは非置換またはモノ −若しくはポリ−置換シクロペンタジエニル基であり、Mはメタロセン−形成金 属原子であり、そしてA及びBは同一であっても異なっていてもよいハロゲン原 子、水素原子、ヒドロキシル基、アルコキシド基若しくはアルキル基を表し、そ してmは1若しくは2、m+n+pはMの原子価に等しい。)である、請求項2 0に記載のカチオン交換樹脂の使用。
Applications Claiming Priority (3)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
US08/118,338 US5455214A (en) | 1993-09-09 | 1993-09-09 | Metallocenes supported on ion exchange resins |
US118,338 | 1993-09-09 | ||
PCT/US1994/009970 WO1995007140A1 (en) | 1993-09-09 | 1994-09-06 | Catalyst precursor composition, and method of making the same |
Publications (2)
Publication Number | Publication Date |
---|---|
JPH09505511A true JPH09505511A (ja) | 1997-06-03 |
JP3950921B2 JP3950921B2 (ja) | 2007-08-01 |
Family
ID=22377959
Family Applications (1)
Application Number | Title | Priority Date | Filing Date |
---|---|---|---|
JP50874895A Expired - Fee Related JP3950921B2 (ja) | 1993-09-09 | 1994-09-06 | 触媒前駆体組成物、及びその製造方法 |
Country Status (8)
Country | Link |
---|---|
US (1) | US5455214A (ja) |
EP (1) | EP0717660B1 (ja) |
JP (1) | JP3950921B2 (ja) |
KR (1) | KR960704631A (ja) |
AU (1) | AU688386B2 (ja) |
CA (1) | CA2169074C (ja) |
DE (1) | DE69431156T2 (ja) |
WO (1) | WO1995007140A1 (ja) |
Families Citing this family (22)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
IT1264680B1 (it) * | 1993-07-07 | 1996-10-04 | Spherilene Srl | Catalizzatori supportati per la polimerizzazione delle olefine |
EP0727443B1 (en) * | 1995-02-20 | 2001-01-17 | Tosoh Corporation | Catalyst for olefin polymerization and process for producing olefin polymers |
US5885924A (en) * | 1995-06-07 | 1999-03-23 | W. R. Grace & Co.-Conn. | Halogenated supports and supported activators |
DK0863919T3 (da) * | 1995-11-27 | 2000-12-11 | Grace W R & Co | Understøttet katalysator indeholdende en tøjret, kationdannende aktivator |
DE69720823T2 (de) | 1996-01-25 | 2004-01-22 | Tosoh Corp., Shinnanyo | Verfahren zur Olefinpolymerisierung unter Verwendung eines Übergangsmetallkatalysators. |
GB9613814D0 (en) * | 1996-07-02 | 1996-09-04 | Bp Chem Int Ltd | Supported polymerisation catalysts |
EP0978499B2 (en) * | 1996-07-23 | 2010-05-05 | Symyx Solutions Inc. | Combinatorial synthesis and analysis of organometallic compounds and catalysts |
US6339134B1 (en) | 1999-05-06 | 2002-01-15 | Univation Technologies, Llc | Polymerization process for producing easier processing polymers |
US6281306B1 (en) | 1999-12-16 | 2001-08-28 | Univation Technologies, Llc | Method of polymerization |
US6524987B1 (en) * | 1999-12-22 | 2003-02-25 | Phillips Petroleum Company | Organometal catalyst compositions |
JP2002003659A (ja) * | 2000-06-21 | 2002-01-09 | Toyo Ink Mfg Co Ltd | 着色樹脂組成物および成形品 |
NO20013880L (no) | 2000-08-22 | 2002-02-25 | Rohm & Haas | Matriks og fremgangsmåte for fremstilling av polyolefiner |
US7074736B2 (en) * | 2000-10-31 | 2006-07-11 | Rohm And Haas Company | Hydrozirconated matrix and process for polyolefin production |
WO2004046214A2 (en) | 2002-10-15 | 2004-06-03 | Exxonmobil Chemical Patents Inc. | Multiple catalyst system for olefin polymerization and polymers produced therefrom |
US7223822B2 (en) | 2002-10-15 | 2007-05-29 | Exxonmobil Chemical Patents Inc. | Multiple catalyst and reactor system for olefin polymerization and polymers produced therefrom |
WO2004094487A1 (en) | 2003-03-21 | 2004-11-04 | Dow Global Technologies, Inc. | Morphology controlled olefin polymerization process |
EP1803747A1 (en) | 2005-12-30 | 2007-07-04 | Borealis Technology Oy | Surface-modified polymerization catalysts for the preparation of low-gel polyolefin films |
TW200932762A (en) | 2007-10-22 | 2009-08-01 | Univation Tech Llc | Polyethylene compositions having improved properties |
CN101939343B (zh) | 2007-12-18 | 2013-10-02 | 尤尼威蒂恩技术有限责任公司 | 聚合期间控制双峰催化剂活性的方法 |
SG11201703851UA (en) | 2014-11-25 | 2017-06-29 | Univation Tech Llc | Methods of controlling polyolefin melt index |
EP4330294A1 (en) | 2021-04-30 | 2024-03-06 | ExxonMobil Chemical Patents Inc. | Processes for transitioning between different polymerization catalysts in a polymerization reactor |
CN117683310B (zh) * | 2024-02-02 | 2024-04-30 | 国家电投集团氢能科技发展有限公司 | 一种复合物、离子交换膜及其制备方法和应用 |
Family Cites Families (4)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
US4111856A (en) * | 1972-11-15 | 1978-09-05 | Mobil Oil Corporation | Insoluble resin-metal compound complex prepared by contacting weak base ion exchange resin with solution of metal-ligand |
US5198401A (en) * | 1987-01-30 | 1993-03-30 | Exxon Chemical Patents Inc. | Ionic metallocene catalyst compositions |
CA2027145C (en) * | 1989-10-10 | 2002-12-10 | Michael J. Elder | Metallocene catalysts with lewis acids and aluminum alkyls |
DE69222317T2 (de) * | 1991-11-25 | 1998-02-12 | Exxon Chemical Patents Inc | Polyionische, uebergangsmetall enthaltende katalysatorzusammensetzung |
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1993
- 1993-09-09 US US08/118,338 patent/US5455214A/en not_active Expired - Lifetime
-
1994
- 1994-09-06 EP EP94929138A patent/EP0717660B1/en not_active Expired - Lifetime
- 1994-09-06 WO PCT/US1994/009970 patent/WO1995007140A1/en active IP Right Grant
- 1994-09-06 JP JP50874895A patent/JP3950921B2/ja not_active Expired - Fee Related
- 1994-09-06 AU AU78310/94A patent/AU688386B2/en not_active Ceased
- 1994-09-06 CA CA002169074A patent/CA2169074C/en not_active Expired - Fee Related
- 1994-09-06 DE DE69431156T patent/DE69431156T2/de not_active Expired - Fee Related
- 1994-09-06 KR KR1019960701153A patent/KR960704631A/ko not_active Application Discontinuation
Also Published As
Publication number | Publication date |
---|---|
WO1995007140A1 (en) | 1995-03-16 |
EP0717660A1 (en) | 1996-06-26 |
AU688386B2 (en) | 1998-03-12 |
US5455214A (en) | 1995-10-03 |
AU7831094A (en) | 1995-03-27 |
EP0717660A4 (en) | 1997-11-12 |
JP3950921B2 (ja) | 2007-08-01 |
EP0717660B1 (en) | 2002-08-07 |
DE69431156T2 (de) | 2002-12-05 |
CA2169074C (en) | 2006-10-24 |
DE69431156D1 (de) | 2002-09-12 |
KR960704631A (ko) | 1996-10-09 |
CA2169074A1 (en) | 1995-03-16 |
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