KR900012963A - 유리-말단 장측쇄를 가진 프로필렌 중합체의 제조방법 및 이의 용도 - Google Patents
유리-말단 장측쇄를 가진 프로필렌 중합체의 제조방법 및 이의 용도 Download PDFInfo
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- KR900012963A KR900012963A KR1019900001982A KR900001982A KR900012963A KR 900012963 A KR900012963 A KR 900012963A KR 1019900001982 A KR1019900001982 A KR 1019900001982A KR 900001982 A KR900001982 A KR 900001982A KR 900012963 A KR900012963 A KR 900012963A
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- propylene polymer
- temperature
- peroxide
- polymer material
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- 229920001155 polypropylene Polymers 0.000 title claims 35
- 238000004519 manufacturing process Methods 0.000 title claims 3
- 238000000034 method Methods 0.000 claims 28
- 238000000354 decomposition reaction Methods 0.000 claims 22
- 150000002978 peroxides Chemical class 0.000 claims 22
- 239000002861 polymer material Substances 0.000 claims 22
- 239000007787 solid Substances 0.000 claims 11
- 239000011521 glass Substances 0.000 claims 10
- -1 polypropylene Polymers 0.000 claims 10
- 239000000203 mixture Substances 0.000 claims 8
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 claims 6
- 239000007789 gas Substances 0.000 claims 6
- 229910052760 oxygen Inorganic materials 0.000 claims 6
- 239000001301 oxygen Substances 0.000 claims 6
- 238000002156 mixing Methods 0.000 claims 4
- 239000004743 Polypropylene Substances 0.000 claims 3
- 238000010128 melt processing Methods 0.000 claims 3
- 238000005482 strain hardening Methods 0.000 claims 3
- HGXJDMCMYLEZMJ-UHFFFAOYSA-N (2-methylpropan-2-yl)oxy 2,2-dimethylpropaneperoxoate Chemical compound CC(C)(C)OOOC(=O)C(C)(C)C HGXJDMCMYLEZMJ-UHFFFAOYSA-N 0.000 claims 2
- YKTNISGZEGZHIS-UHFFFAOYSA-N 2-$l^{1}-oxidanyloxy-2-methylpropane Chemical group CC(C)(C)O[O] YKTNISGZEGZHIS-UHFFFAOYSA-N 0.000 claims 2
- 238000007792 addition Methods 0.000 claims 2
- BSJPKCJHTSQKHH-UHFFFAOYSA-N butan-2-yl butan-2-yloxycarbonyloxyperoxy carbonate Chemical group CCC(C)OC(=O)OOOOC(=O)OC(C)CC BSJPKCJHTSQKHH-UHFFFAOYSA-N 0.000 claims 2
- ZGPBOPXFOJBLIV-UHFFFAOYSA-N butoxycarbonyloxy butyl carbonate Chemical compound CCCCOC(=O)OOC(=O)OCCCC ZGPBOPXFOJBLIV-UHFFFAOYSA-N 0.000 claims 2
- BSQKFIMWHXZMPC-UHFFFAOYSA-N ethylperoxyperoxyethane Chemical group CCOOOOCC BSQKFIMWHXZMPC-UHFFFAOYSA-N 0.000 claims 2
- 238000013467 fragmentation Methods 0.000 claims 2
- 238000006062 fragmentation reaction Methods 0.000 claims 2
- 238000010438 heat treatment Methods 0.000 claims 2
- BWJUFXUULUEGMA-UHFFFAOYSA-N propan-2-yl propan-2-yloxycarbonyloxy carbonate Chemical compound CC(C)OC(=O)OOC(=O)OC(C)C BWJUFXUULUEGMA-UHFFFAOYSA-N 0.000 claims 2
- YPVDWEHVCUBACK-UHFFFAOYSA-N propoxycarbonyloxy propyl carbonate Chemical compound CCCOC(=O)OOC(=O)OCCC YPVDWEHVCUBACK-UHFFFAOYSA-N 0.000 claims 2
- 239000007858 starting material Substances 0.000 claims 2
- KDGNCLDCOVTOCS-UHFFFAOYSA-N (2-methylpropan-2-yl)oxy propan-2-yl carbonate Chemical compound CC(C)OC(=O)OOC(C)(C)C KDGNCLDCOVTOCS-UHFFFAOYSA-N 0.000 claims 1
- HSLFISVKRDQEBY-UHFFFAOYSA-N 1,1-bis(tert-butylperoxy)cyclohexane Chemical compound CC(C)(C)OOC1(OOC(C)(C)C)CCCCC1 HSLFISVKRDQEBY-UHFFFAOYSA-N 0.000 claims 1
- DMWVYCCGCQPJEA-UHFFFAOYSA-N 2,5-bis(tert-butylperoxy)-2,5-dimethylhexane Chemical group CC(C)(C)OOC(C)(C)CCC(C)(C)OOC(C)(C)C DMWVYCCGCQPJEA-UHFFFAOYSA-N 0.000 claims 1
- XMNIXWIUMCBBBL-UHFFFAOYSA-N 2-(2-phenylpropan-2-ylperoxy)propan-2-ylbenzene Chemical compound C=1C=CC=CC=1C(C)(C)OOC(C)(C)C1=CC=CC=C1 XMNIXWIUMCBBBL-UHFFFAOYSA-N 0.000 claims 1
- CARSMBZECAABMO-UHFFFAOYSA-N 3-chloro-2,6-dimethylbenzoic acid Chemical compound CC1=CC=C(Cl)C(C)=C1C(O)=O CARSMBZECAABMO-UHFFFAOYSA-N 0.000 claims 1
- OAICVXFJPJFONN-UHFFFAOYSA-N Phosphorus Chemical compound [P] OAICVXFJPJFONN-UHFFFAOYSA-N 0.000 claims 1
- WPYMKLBDIGXBTP-UHFFFAOYSA-N benzoic acid Chemical compound OC(=O)C1=CC=CC=C1 WPYMKLBDIGXBTP-UHFFFAOYSA-N 0.000 claims 1
- 238000001879 gelation Methods 0.000 claims 1
- 239000000463 material Substances 0.000 claims 1
- 238000002844 melting Methods 0.000 claims 1
- 230000008018 melting Effects 0.000 claims 1
- DSXJYGUJWPLXKE-UHFFFAOYSA-N pentoxy 7,7-dimethyloctaneperoxoate Chemical compound CCCCCOOOC(=O)CCCCCC(C)(C)C DSXJYGUJWPLXKE-UHFFFAOYSA-N 0.000 claims 1
- 229910052698 phosphorus Inorganic materials 0.000 claims 1
- 239000011574 phosphorus Substances 0.000 claims 1
- 239000000843 powder Substances 0.000 claims 1
- 238000003672 processing method Methods 0.000 claims 1
- GJBRNHKUVLOCEB-UHFFFAOYSA-N tert-butyl benzenecarboperoxoate Chemical compound CC(C)(C)OOC(=O)C1=CC=CC=C1 GJBRNHKUVLOCEB-UHFFFAOYSA-N 0.000 claims 1
- 125000000999 tert-butyl group Chemical group [H]C([H])([H])C(*)(C([H])([H])[H])C([H])([H])[H] 0.000 claims 1
- 239000013068 control sample Substances 0.000 description 1
Classifications
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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
- C08F8/00—Chemical modification by after-treatment
- C08F8/50—Partial depolymerisation
-
- 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
- C08F230/00—Copolymers of compounds having one or more unsaturated aliphatic radicals, each having only one carbon-to-carbon double bond, and containing phosphorus, selenium, tellurium or a metal
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- Chemical & Material Sciences (AREA)
- Health & Medical Sciences (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Medicinal Chemistry (AREA)
- Polymers & Plastics (AREA)
- Organic Chemistry (AREA)
- General Chemical & Material Sciences (AREA)
- Addition Polymer Or Copolymer, Post-Treatments, Or Chemical Modifications (AREA)
- Artificial Filaments (AREA)
- Compositions Of Macromolecular Compounds (AREA)
- Manufacture Of Macromolecular Shaped Articles (AREA)
- Materials For Medical Uses (AREA)
- Medicines Containing Antibodies Or Antigens For Use As Internal Diagnostic Agents (AREA)
- Processes Of Treating Macromolecular Substances (AREA)
Abstract
Description
Claims (28)
- (1) 저분해 온도 과산화물을 대기 산소 또는 이와 유사한 기체의 실질적인 부재하 혼합 용기내에서 실온 내지 120℃하의 직쇄 프로필렌 중합체 물질과 혼합하고, (2) 과산화물의 분해가 일어나고 상당량의 직쇄 프로필렌 중합체 물질의 단편화가 일어나며 상당량의 장측쇄가 형성되기엔 충분한 시간이지만 프로필렌 중합체 물질의 겔화가 일어나기엔 불충분한 시간 동안 실온 내지 120℃에서 대기 산소 또는 이와 유사한 기체의 실질적인 부재하에 생성된 혼합물을 가열 또는 유지시키며, (3) 대기 산소 또는 이와 유사한 기체의 실질적인 부재하에 프로필렌 중합체 물질을 처리하여 상기 프로필렌 중합체 물질에 존재하는 실질적으로 모든 자유 라디칼을 탈활성시킴을 특징으로 하여, 변형 경화 신장 점도가 없는, 통상적으로 고체인 무정형 내지 우세한 결정성 프로필렌 중합체 물질로부터 1미만의 분지 지수 및 변형 경화 신장점도를 가진 통상적으로 고체인, 겔-유리, 프로필렌중합체 물질을 제조하는 방법.
- 제1항에 있어서, 상기 무정형 내지 우세한 결정성 프로필렌 중합체 물질이 통상적으로 고체인, 겔-유리, 우세한 이소택틱, 반결정성 폴리프로필렌인 방법.
- 제1항에 있어서, 저분해 온도 과산화물의 반감기가 약 90℃내지 120℃의 온도범위에서 5분이하, 또는 약 60℃ 내지 약 90℃의 온도 범위에서 40분 미만, 또는 실온 내지 약 60℃의 온도범위에서 60분 미만의 방법.
- 제3항에 있어서, 저분해 온도 과산화물을 디(2급-부틸)퍼옥시 디카보네이트, 비스(2-에톡시)-퍼옥시 디카보네이트, 디-사이클로헥실퍼옥시 디카보네이트, 디-n-프로필-퍼옥시 디카보네이트, 디-n-부틸퍼옥시 디카보네이트, 디-2급-부틸퍼옥시 디카보네이트, 디-이소프로필퍼옥시 디카보네이트, 3급-부틸퍼옥시 네오테카노에이트, 3급-아밀퍼옥시 네오데카노에이트 및 3급-부틸 퍼옥시 피발레이트중에서 선택하는 방법.
- 제1항에 있어서, 저분해 온도 과산화물의 반감기가 단계(2)에서 사용된 온도에서 약 10초 내지 약 5분인 방법.
- 제1항에 있어서, 단계(2)의 온도가 60 내지 110℃인 방법.
- 제1항에 있어서, 온도가 70 내지 105℃인 방법.
- 제1항에 있어서, 저분해 온도 과산화물의 농도가 0.005 내지 0.05㎜oles/g 프로필렌 중합체 출발물질인 방법.
- 제3항에 있어서, 저분해 온도 과산화물의 농도가 0.005 내지 0.05㎜oles/g 프로필렌 중합체 출발물질인 방법.
- 제1항에 있어서, 프로필렌 중합체 물질을 저분해 온도 과산화물 첨가전 20초 이상동안 단계(2)에서 사용한 온도하에 유지시키는 방법.
- (1) 저분해 온도 과산화물 및 고분해 온도 과산화물을 대기 산소 또는 이와 유사한 기체의 실질적인 부재하 혼합용기내에서 실온 내지 120℃이하의 직쇄 프로필렌 중합체 물질과 혼합하고, (2) 저분재 온도 과산화물의 분해가 일어나고 직쇄 프로필렌 중합체 물질의 실질적인 양의 단편화가 일어나며 상당량의 장측쇄가 형성되기엔 충분한 시간이지만 프로필렌 중합체 물질의 겔화가 일어나기엔 불충분한 시간 동안 실온 내지 120℃에서 대기 산소 또는 이와 유사한 기체의 실질적인 부재하에 생성된 혼합물을 가열 또는 유지시키며, (3)대기 산소 또는 이와 유사한 기체의 실질적인 부재하에 프로필렌 중합체 물질을 처리하여, 저분해 온도 과산화물로부터 수득된 상기 프로필렌 중합체 물질에 존재하는 실질적으로 모든 자유 라디칼을 탈활성시키고, 고분해 온도 과산화물을 분해시킨후 고분해 온도 과산화물로부터 수득된 상기 프로필렌 중합체 물질에 존재하는 잔류 자유 라디칼을 탈활성화시킴을 특징으로 하여, 변형 경화 신장 점도가 없는, 통상적으로 고체인 무정형 내지 우세한 결정성 프로필렌 중합체 물질로부터 1미만의 분지지수 및 변형 경화 신장 점도를 가진 통상적으로 고체인, 겔-유리, 프로필렌 중합체 물질을 제조하는 방법.
- 제11항에 있어서, 상기 부정형 내지 우세한 결정성 폴리프로필렌이 통상적으로 고체인, 겔-유리, 우세한 이소택틱, 반결정성 폴리프로필렌인 방법.
- 제11항에 있어서, 저분해온도과산화물을 디(2급-부틸)퍼옥시 디카보네이트, 비스(2-에톡시)-퍼옥시 디카보네이트, 디-사이클로헥실퍼옥시 디카보네이트, 디-n-프로필퍼옥시 디카보네이트, 디-n-부틸퍼옥시 디카보네이트, 디-2급-부틸퍼옥시 디카보네이트, 디-이소프로필퍼옥시 디카보네이트, 3급-부틸퍼옥시 네오테카노에이트, 3급-아밀퍼옥시 네오데카노에이트 및 3급-부틸 퍼옥시 피발레이트중에서 선택하는 방법.
- 제11항에 있어서, 고분해온도 과산화물을 2,5-디메틸-2,5-비스(3급-부틸퍼옥시)헥산, 비스(3급-부틸퍼옥시-이소프로필)벤젤, 디쿠밀 퍼옥사이드, 4,4-디-3급-부틸퍼옥시-n-부틸발레에이트, 3급-이밀퍼옥시 벤조에이트, 3급-부틸퍼옥시 벤조에이트, 2,2-디-3급 부틸 퍼옥시부탄, 3급-부틸-퍼옥시-3,5,5-트리메틸 헥사노에이트, 3급-부틸퍼옥시 이소프로필 카보네이트 및 1,1-디-3급 부틸퍼옥시 사이클로헥산중에서 선택하는 방법.
- 제11항에 있어서, 저분해 온도 과산화물의 빈감기가 약 90℃ 내지 120℃의 온도 범위에서 5분 이하, 또는 약 60℃ 내지 약 90℃의 온도 범위에서 40분 미만, 또는 실온 내지 약 60℃의 온도 범위에서 60분 미만이고, 고분해 과산화물의 반감기가 120℃에서 20분 이상, 또는 단계(3)에서 사용한 온도에서 60분 이상인 방법.
- 제15항에 있어서, 저분해 온도 과산화물의 반감기가 단계(2)에서 사용한 온도에서 10초 내지 5분인 방법.
- 제15항에 있어서, 고분해 온도 과산화물의 반감기가 단계(3)에서 사용한 온도에서 30초 내지 약 10분인 방법.
- 제11항에 있어서, 단계(2)의 온도가 60 내지 110℃인 방법.
- 제11항에 있어서, 단계(2)의 온도가 70 내지 105℃인 방법.
- 제11항에 있어서, 단계(3)의 온도가 130°내지 150℃인 방법.
- 제19항에 있어서, 단계(3)의 온도가 140°내지 150℃인 방법.
- 제11항에 있어서, 단계(2)에서 사용한 온도가 저 및 고분해 과산화물 첨가 전 20초 이상 동안 사용되고 유지되는 방법.
- 제1항의 제조방법에 따라 제조된, 분지지수 1미만의 통상적으로 무정형 고체인, 겔-유리 내지 우세한 결정성 프로필렌 중합체 물질을 함유하는 용융가공에 유용한 프로필렌 중합체 조성물.
- 제1항의 제조방법에 따라 제조된, 분지지수 1미만의, 상당량의 통상적으로 고체인 무정형 겔-유리 내지 우세한 결정성 프로필렌 중합체 물질을 함유하는 프로필렌 중합체 조성물로 부터 유용한 제품을 제조하는 개선된 용융 가공법.
- 제1항의 제조방법에 따라 제조된, 분지지수 1미만의, 상당량의 통상적으로 무정형 고체인, 겔-유리 내지 우세한 결정성 프로필렌 중합체 물질을 함유하는 프로필렌 중합체 조성물로 부터 제조된 유용한 제품.
- 제11항의 제조방법에 따라 제조된, 분지지수 1미만의 통상적으로 고체인 무정형 겔-유리 내지 우세한 결정성 프로필렌 중합체 물질을 함유하는, 용융가공에 유용한 프로필렌 중합체 조성물.
- 제11항의 제조방법에 따라 제조된, 분지지수 1미만의, 상당량의 통상적으로 고체인 무정형, 겔-유리 내지 우세한 결정성 프로필렌 중합체 물질을 함유하는 프로필렌 중합체 조성물로 부터 유용한 제품을 제조하는 개선된 용융 가공법.
- 제11항의 제조방법에 따라 제조된, 분지지수 1미만의 상당량의 통상적으로 고체인 무정형, 겔-유리 내지 우세한 결정성 프로필렌 중합체 물질을 함유하는 프로필렌 중합체 조성물로 부터 제조된 유용한 제품.※ 참고사항 : 최초출원 내용에 의하여 공개하는 것임.
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KR900012963A true KR900012963A (ko) | 1990-09-03 |
KR0145323B1 KR0145323B1 (ko) | 1998-07-15 |
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KR1019900001982A KR0145323B1 (ko) | 1989-02-21 | 1990-02-19 | 유리 말단 장측쇄를 갖는 프로필렌 중합체의 제조방법 및 이의 용도 |
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US (1) | US5047485A (ko) |
EP (1) | EP0384431B1 (ko) |
JP (1) | JP2744317B2 (ko) |
KR (1) | KR0145323B1 (ko) |
CN (1) | CN1030457C (ko) |
AT (1) | ATE114677T1 (ko) |
AU (1) | AU616103B2 (ko) |
BR (1) | BR9000791A (ko) |
CA (1) | CA1339476C (ko) |
DE (1) | DE69014348T2 (ko) |
DK (1) | DK0384431T3 (ko) |
ES (1) | ES2064503T3 (ko) |
FI (1) | FI900836A0 (ko) |
NO (1) | NO900738L (ko) |
PT (1) | PT93206A (ko) |
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EP4086299B1 (en) | 2021-05-03 | 2024-07-03 | Borealis AG | Thermally treated biaxially oriented polypropylene film |
EP4491395A1 (en) | 2023-07-10 | 2025-01-15 | Borealis AG | Composition comprising nucleated polypropylene and cyclic olefin polymer for capacitors |
Family Cites Families (12)
Publication number | Priority date | Publication date | Assignee | Title |
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US3144436A (en) * | 1961-01-04 | 1964-08-11 | Du Pont | Process for degrading stereoregular polymers |
JPS5148196B2 (ko) * | 1972-03-11 | 1976-12-18 | ||
US4451589A (en) * | 1981-06-15 | 1984-05-29 | Kimberly-Clark Corporation | Method of improving processability of polymers and resulting polymer compositions |
FR2508047B1 (fr) * | 1981-06-22 | 1985-10-11 | Bp Chimie Sa | Procede de traitement de polyethylene de basse densite lineaire par des peroxydes organiques, generateurs de radicaux libres |
US4378451A (en) * | 1981-09-14 | 1983-03-29 | Eastman Kodak Company | High flow rate polyolefin extrusion coating compositions |
FR2562546B1 (fr) * | 1984-04-09 | 1987-01-23 | Bp Chimie Sa | Procede de traitement de polyethylene de basse densite lineaire destine a la fabrication par extrusion de corps creux, tubes et gaines |
US4578430A (en) * | 1984-12-19 | 1986-03-25 | Shell Oil Company | Controlled degradation or cracking of alpha-olefin polymers |
US4707524A (en) * | 1986-05-06 | 1987-11-17 | Aristech Chemical Corporation | Controlled-rheology polypropylene |
GB8620502D0 (en) * | 1986-08-22 | 1986-10-01 | Du Pont Canada | Modification of crystalline propylene polymers |
FR2613722B1 (fr) * | 1987-04-07 | 1990-11-23 | Bp Chimie Sa | Procede de fabrication de granules d'homopolymere ou de copolymere de propylene |
NO172497C (no) * | 1987-12-14 | 1993-07-28 | Akzo Nv | Fremgangsmaate formodifikasjon av (ko)polymerer ved anvendelse av organiske peroksyder og anvendelse av disse |
WO1991000301A1 (en) * | 1989-06-28 | 1991-01-10 | Akzo N.V. | (CO)POLYMER MODIFICATION EMPLOYING UNSATURATED t-ALKYL PEROXYALKENYL CARBONATES |
-
1989
- 1989-02-21 US US07/313,274 patent/US5047485A/en not_active Expired - Lifetime
- 1989-09-25 CA CA000613067A patent/CA1339476C/en not_active Expired - Fee Related
-
1990
- 1990-02-07 ZA ZA90911A patent/ZA90911B/xx unknown
- 1990-02-15 NO NO90900738A patent/NO900738L/no unknown
- 1990-02-16 RU SU904743214A patent/RU2036931C1/ru active
- 1990-02-19 KR KR1019900001982A patent/KR0145323B1/ko not_active IP Right Cessation
- 1990-02-19 AU AU49943/90A patent/AU616103B2/en not_active Ceased
- 1990-02-20 JP JP2039540A patent/JP2744317B2/ja not_active Expired - Lifetime
- 1990-02-20 PT PT93206A patent/PT93206A/pt not_active Application Discontinuation
- 1990-02-20 BR BR909000791A patent/BR9000791A/pt not_active IP Right Cessation
- 1990-02-20 FI FI900836A patent/FI900836A0/fi not_active IP Right Cessation
- 1990-02-21 ES ES90103333T patent/ES2064503T3/es not_active Expired - Lifetime
- 1990-02-21 AT AT90103333T patent/ATE114677T1/de not_active IP Right Cessation
- 1990-02-21 EP EP90103333A patent/EP0384431B1/en not_active Expired - Lifetime
- 1990-02-21 DK DK90103333.2T patent/DK0384431T3/da active
- 1990-02-21 CN CN90100952A patent/CN1030457C/zh not_active Expired - Lifetime
- 1990-02-21 DE DE69014348T patent/DE69014348T2/de not_active Expired - Fee Related
Also Published As
Publication number | Publication date |
---|---|
PT93206A (pt) | 1990-08-31 |
CN1045107A (zh) | 1990-09-05 |
EP0384431A3 (en) | 1991-10-09 |
US5047485A (en) | 1991-09-10 |
ES2064503T3 (es) | 1995-02-01 |
AU4994390A (en) | 1990-08-30 |
DE69014348T2 (de) | 1995-04-20 |
AU616103B2 (en) | 1991-10-17 |
BR9000791A (pt) | 1991-01-22 |
JP2744317B2 (ja) | 1998-04-28 |
DK0384431T3 (da) | 1995-01-16 |
EP0384431A2 (en) | 1990-08-29 |
EP0384431B1 (en) | 1994-11-30 |
ZA90911B (en) | 1990-12-28 |
NO900738L (no) | 1990-08-22 |
JPH02298536A (ja) | 1990-12-10 |
CN1030457C (zh) | 1995-12-06 |
DE69014348D1 (de) | 1995-01-12 |
KR0145323B1 (ko) | 1998-07-15 |
ATE114677T1 (de) | 1994-12-15 |
FI900836A0 (fi) | 1990-02-20 |
NO900738D0 (no) | 1990-02-15 |
CA1339476C (en) | 1997-09-23 |
RU2036931C1 (ru) | 1995-06-09 |
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