KR910016378A - 무수 프탈산 제조용 촉매 - Google Patents
무수 프탈산 제조용 촉매 Download PDFInfo
- Publication number
- KR910016378A KR910016378A KR1019910004158A KR910004158A KR910016378A KR 910016378 A KR910016378 A KR 910016378A KR 1019910004158 A KR1019910004158 A KR 1019910004158A KR 910004158 A KR910004158 A KR 910004158A KR 910016378 A KR910016378 A KR 910016378A
- Authority
- KR
- South Korea
- Prior art keywords
- weight
- parts
- catalyst
- phthalic anhydride
- oxide
- Prior art date
Links
- LGRFSURHDFAFJT-UHFFFAOYSA-N Phthalic anhydride Natural products C1=CC=C2C(=O)OC(=O)C2=C1 LGRFSURHDFAFJT-UHFFFAOYSA-N 0.000 title claims 6
- JHIWVOJDXOSYLW-UHFFFAOYSA-N butyl 2,2-difluorocyclopropane-1-carboxylate Chemical compound CCCCOC(=O)C1CC1(F)F JHIWVOJDXOSYLW-UHFFFAOYSA-N 0.000 title claims 6
- 239000003054 catalyst Substances 0.000 title claims 6
- MYMOFIZGZYHOMD-UHFFFAOYSA-N Dioxygen Chemical compound O=O MYMOFIZGZYHOMD-UHFFFAOYSA-N 0.000 claims 4
- UFWIBTONFRDIAS-UHFFFAOYSA-N Naphthalene Chemical compound C1=CC=CC2=CC=CC=C21 UFWIBTONFRDIAS-UHFFFAOYSA-N 0.000 claims 4
- 229910001882 dioxygen Inorganic materials 0.000 claims 4
- 239000011148 porous material Substances 0.000 claims 4
- 239000007789 gas Substances 0.000 claims 3
- CTQNGGLPUBDAKN-UHFFFAOYSA-N O-Xylene Chemical group CC1=CC=CC=C1C CTQNGGLPUBDAKN-UHFFFAOYSA-N 0.000 claims 2
- OAICVXFJPJFONN-UHFFFAOYSA-N Phosphorus Chemical compound [P] OAICVXFJPJFONN-UHFFFAOYSA-N 0.000 claims 2
- ZLMJMSJWJFRBEC-UHFFFAOYSA-N Potassium Chemical compound [K] ZLMJMSJWJFRBEC-UHFFFAOYSA-N 0.000 claims 2
- 229910010413 TiO 2 Inorganic materials 0.000 claims 2
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 claims 2
- XHCLAFWTIXFWPH-UHFFFAOYSA-N [O-2].[O-2].[O-2].[O-2].[O-2].[V+5].[V+5] Chemical compound [O-2].[O-2].[O-2].[O-2].[O-2].[V+5].[V+5] XHCLAFWTIXFWPH-UHFFFAOYSA-N 0.000 claims 2
- 239000011149 active material Substances 0.000 claims 2
- 229910052787 antimony Inorganic materials 0.000 claims 2
- WATWJIUSRGPENY-UHFFFAOYSA-N antimony atom Chemical compound [Sb] WATWJIUSRGPENY-UHFFFAOYSA-N 0.000 claims 2
- 229910052758 niobium Inorganic materials 0.000 claims 2
- 239000010955 niobium Substances 0.000 claims 2
- GUCVJGMIXFAOAE-UHFFFAOYSA-N niobium atom Chemical compound [Nb] GUCVJGMIXFAOAE-UHFFFAOYSA-N 0.000 claims 2
- 230000003647 oxidation Effects 0.000 claims 2
- 238000007254 oxidation reaction Methods 0.000 claims 2
- 229910052698 phosphorus Inorganic materials 0.000 claims 2
- 239000011574 phosphorus Substances 0.000 claims 2
- 229910052700 potassium Inorganic materials 0.000 claims 2
- 239000011591 potassium Substances 0.000 claims 2
- BKVIYDNLLOSFOA-UHFFFAOYSA-N thallium Chemical compound [Tl] BKVIYDNLLOSFOA-UHFFFAOYSA-N 0.000 claims 2
- 229910052716 thallium Inorganic materials 0.000 claims 2
- 229910001935 vanadium oxide Inorganic materials 0.000 claims 2
- FAWNVSNJFDIJRM-UHFFFAOYSA-N [Rb].[Cs] Chemical compound [Rb].[Cs] FAWNVSNJFDIJRM-UHFFFAOYSA-N 0.000 claims 1
- 239000013543 active substance Substances 0.000 claims 1
- 229910052792 caesium Inorganic materials 0.000 claims 1
- TVFDJXOCXUVLDH-UHFFFAOYSA-N caesium atom Chemical compound [Cs] TVFDJXOCXUVLDH-UHFFFAOYSA-N 0.000 claims 1
- 239000012071 phase Substances 0.000 claims 1
- 229910052701 rubidium Inorganic materials 0.000 claims 1
- IGLNJRXAVVLDKE-UHFFFAOYSA-N rubidium atom Chemical compound [Rb] IGLNJRXAVVLDKE-UHFFFAOYSA-N 0.000 claims 1
- 229910052709 silver Inorganic materials 0.000 claims 1
- 239000004332 silver Substances 0.000 claims 1
- XOLBLPGZBRYERU-UHFFFAOYSA-N tin dioxide Chemical compound O=[Sn]=O XOLBLPGZBRYERU-UHFFFAOYSA-N 0.000 claims 1
- 229910001887 tin oxide Inorganic materials 0.000 claims 1
- OGIDPMRJRNCKJF-UHFFFAOYSA-N titanium oxide Inorganic materials [Ti]=O OGIDPMRJRNCKJF-UHFFFAOYSA-N 0.000 claims 1
- 239000012808 vapor phase Substances 0.000 claims 1
Classifications
-
- 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
- B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
- B01J23/16—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of arsenic, antimony, bismuth, vanadium, niobium, tantalum, polonium, chromium, molybdenum, tungsten, manganese, technetium or rhenium
- B01J23/20—Vanadium, niobium or tantalum
- B01J23/22—Vanadium
-
- 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
- B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
- B01J23/002—Mixed oxides other than spinels, e.g. perovskite
-
- 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
- B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
- B01J23/38—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals
- B01J23/54—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals combined with metals, oxides or hydroxides provided for in groups B01J23/02 - B01J23/36
- B01J23/66—Silver or gold
- B01J23/68—Silver or gold with arsenic, antimony, bismuth, vanadium, niobium, tantalum, polonium, chromium, molybdenum, tungsten, manganese, technetium or rhenium
- B01J23/682—Silver or gold with arsenic, antimony, bismuth, vanadium, niobium, tantalum, polonium, chromium, molybdenum, tungsten, manganese, technetium or rhenium with vanadium, niobium, tantalum or polonium
-
- 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
- B01J27/00—Catalysts comprising the elements or compounds of halogens, sulfur, selenium, tellurium, phosphorus or nitrogen; Catalysts comprising carbon compounds
- B01J27/14—Phosphorus; Compounds thereof
- B01J27/16—Phosphorus; Compounds thereof containing oxygen, i.e. acids, anhydrides and their derivates with N, S, B or halogens without carriers or on carriers based on C, Si, Al or Zr; also salts of Si, Al and Zr
- B01J27/18—Phosphorus; Compounds thereof containing oxygen, i.e. acids, anhydrides and their derivates with N, S, B or halogens without carriers or on carriers based on C, Si, Al or Zr; also salts of Si, Al and Zr with metals other than Al or Zr
- B01J27/1802—Salts or mixtures of anhydrides with compounds of other metals than V, Nb, Ta, Cr, Mo, W, Mn, Tc, Re, e.g. phosphates, thiophosphates
- B01J27/1817—Salts or mixtures of anhydrides with compounds of other metals than V, Nb, Ta, Cr, Mo, W, Mn, Tc, Re, e.g. phosphates, thiophosphates with copper, silver or gold
-
- 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
- B01J27/00—Catalysts comprising the elements or compounds of halogens, sulfur, selenium, tellurium, phosphorus or nitrogen; Catalysts comprising carbon compounds
- B01J27/14—Phosphorus; Compounds thereof
- B01J27/186—Phosphorus; Compounds thereof with arsenic, antimony, bismuth, vanadium, niobium, tantalum, polonium, chromium, molybdenum, tungsten, manganese, technetium or rhenium
- B01J27/195—Phosphorus; Compounds thereof with arsenic, antimony, bismuth, vanadium, niobium, tantalum, polonium, chromium, molybdenum, tungsten, manganese, technetium or rhenium with vanadium, niobium or tantalum
- B01J27/198—Vanadium
-
- 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
- B01J35/00—Catalysts, in general, characterised by their form or physical properties
- B01J35/60—Catalysts, in general, characterised by their form or physical properties characterised by their surface properties or porosity
- B01J35/66—Pore distribution
-
- C—CHEMISTRY; METALLURGY
- C07—ORGANIC CHEMISTRY
- C07C—ACYCLIC OR CARBOCYCLIC COMPOUNDS
- C07C51/00—Preparation of carboxylic acids or their salts, halides or anhydrides
- C07C51/16—Preparation of carboxylic acids or their salts, halides or anhydrides by oxidation
- C07C51/21—Preparation of carboxylic acids or their salts, halides or anhydrides by oxidation with molecular oxygen
- C07C51/255—Preparation of carboxylic acids or their salts, halides or anhydrides by oxidation with molecular oxygen of compounds containing six-membered aromatic rings without ring-splitting
- C07C51/265—Preparation of carboxylic acids or their salts, halides or anhydrides by oxidation with molecular oxygen of compounds containing six-membered aromatic rings without ring-splitting having alkyl side chains which are oxidised to carboxyl groups
-
- C—CHEMISTRY; METALLURGY
- C07—ORGANIC CHEMISTRY
- C07C—ACYCLIC OR CARBOCYCLIC COMPOUNDS
- C07C51/00—Preparation of carboxylic acids or their salts, halides or anhydrides
- C07C51/16—Preparation of carboxylic acids or their salts, halides or anhydrides by oxidation
- C07C51/31—Preparation of carboxylic acids or their salts, halides or anhydrides by oxidation of cyclic compounds with ring-splitting
- C07C51/313—Preparation of carboxylic acids or their salts, halides or anhydrides by oxidation of cyclic compounds with ring-splitting with molecular oxygen
-
- 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
- B01J2523/00—Constitutive chemical elements of heterogeneous catalysts
Landscapes
- Chemical & Material Sciences (AREA)
- Organic Chemistry (AREA)
- Engineering & Computer Science (AREA)
- Materials Engineering (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Oil, Petroleum & Natural Gas (AREA)
- Catalysts (AREA)
- Furan Compounds (AREA)
Abstract
내용 없음
Description
본 내용은 요부공개 건이므로 전문내용을 수록하지 않았음
Claims (3)
- 오르토크셀렌 및/또는 나트탈렌을 분자형상의 산소 또는 분자형상의 산소함유가스에 의해 기상접촉 산화하여 무수 프탈산을 제조하기 위한 촉매에 있어서, 산화바나듐을 V2O5로서 1~20중량부, 비표면적이 10~60㎡/g인 아나타아제형 산화티난을 TiO2로서 99~80중량부, 게다가 이들의 2성분의 합계 100중량부 당 칼륨, 세슘, 루비듐 및 탈륨으로부터 선택되는 최소한도 1종의 원소를 산화물로서 0.05~1.2중량부 및 은을 Ag2O로서 0.05~2중량부를 함유하는 촉매활성물질을 내열성 무기질 담체에 담지하여 이루어지는 것을 특징으로 하는 무수 프탈산 제조용 촉매.
- 오르토크실렌 및/또는 나프탈렌을 분자형상의 산소 또는 분자형상의 산소함유가스엔 의해 기상접촉 산화하여 무수 프탈산을 제조하기 위한 촉매에 있어서, 산화바나듐을 V2O5로서, 1~20중량부, 비표면적이 10~60㎡/g 아나타아제형 산화티탄을 TiO2로서 99~80중량부, 게다가 이들 2성분과 함께 100중량부 당 니오브률 Nb2O5로서 0-1중량부, 칼륨, 세슘 루비듐 및 탈륨으로부터 선택되는 최소한도 1종의 원소를 산화물로서 0.05~1.2중량부, 인을 P205로서 0~1.2중량부, 안티몬을 Sb2O3로서 0~5중량부 및 은을 Ag2O로서 0.05~2중량부(단, 니오브, 인 및 안티몬의 각각의 함유량이 동시에 0으로 되는 것은 아님.)를 함유하는 촉매활동성물질을 내열성 무기질 담체에 담지하여 이루어지는 것을 특징으로 하는 무수 프탈산 제조용 촉매.
- 제1항 또는 제2항에 있어서, 내열성 무기질 담체에 담지한 촉매활성 물질층은 0.15~0.45㎛의 직경을 갖는 세공이 차지하는 함께 세공용적이 10㎛이하의 직격을 갖는 세공이 차지하는 전체 세공 용적의 50%이상으로 되어 있는 무수 프탈산 제조용 촉매.※ 참고사항 : 최초출원 내용에 의하여 공개하는 것임.
Applications Claiming Priority (3)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
JP2-63975 | 1990-03-16 | ||
JP?2-063975 | 1990-03-16 | ||
JP6397590 | 1990-03-16 |
Publications (2)
Publication Number | Publication Date |
---|---|
KR910016378A true KR910016378A (ko) | 1991-11-05 |
KR950008197B1 KR950008197B1 (ko) | 1995-07-26 |
Family
ID=13244794
Family Applications (1)
Application Number | Title | Priority Date | Filing Date |
---|---|---|---|
KR1019910004158A KR950008197B1 (ko) | 1990-03-16 | 1991-03-15 | 무수 프탈산 제조용 촉매 |
Country Status (10)
Country | Link |
---|---|
US (1) | US5169820A (ko) |
EP (1) | EP0447267B1 (ko) |
KR (1) | KR950008197B1 (ko) |
CN (1) | CN1024092C (ko) |
AT (1) | ATE106278T1 (ko) |
AU (1) | AU641987B2 (ko) |
BR (1) | BR9101046A (ko) |
DE (1) | DE69102169T2 (ko) |
ES (1) | ES2054441T3 (ko) |
RU (1) | RU2047351C1 (ko) |
Families Citing this family (24)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
US5235071A (en) * | 1991-07-10 | 1993-08-10 | Nippon Shokubai Co., Ltd. | Catalyst for producing phthalic anhydride and process by using the same |
DE59605306D1 (de) * | 1995-03-15 | 2000-06-29 | Basf Ag | Verfahren zur herstellung von phosphordotierten silberkatalysatoren |
US5736483A (en) * | 1996-10-25 | 1998-04-07 | Scientific Design Co., Inc. | Niobium or tantalum promoted silver catalyst |
DE19707943C2 (de) * | 1997-02-27 | 1999-07-08 | Basf Ag | Verfahren zur Herstellung von Phthalsäureanhydrid und Katalysator hierfür |
DE19851786A1 (de) | 1998-11-10 | 2000-05-11 | Basf Ag | Silber- und Vanadiumoxid enthaltendes Multimetalloxid und dessen Verwendung |
DE10022103A1 (de) * | 2000-05-08 | 2001-11-15 | Basf Ag | Silber, Vanadium und ein oder mehrere Elemente der Phosphorgruppe enthaltendes Multimetalloxid und dessen Verwendung |
ZA200200049B (en) * | 2001-01-25 | 2002-07-16 | Nippon Catalytic Chem Ind | Fixed-bed shell-and-tube reactor and its usage. |
US6657068B2 (en) | 2002-03-22 | 2003-12-02 | General Electric Company | Liquid phase oxidation of halogenated ortho-xylenes |
US6657067B2 (en) | 2002-03-22 | 2003-12-02 | General Electric Company | Method for the manufacture of chlorophthalic anhydride |
US6649773B2 (en) | 2002-03-22 | 2003-11-18 | General Electric Company | Method for the manufacture of halophthalic acids and anhydrides |
KR100549777B1 (ko) * | 2002-03-28 | 2006-02-06 | 한국전력기술 주식회사 | 넓은 활성온도 대역을 갖는 질소산화물 및/또는 다이옥신제거용 삼산화 바나듐을 포함한 바나듐/티타니아계 촉매 |
DE10323461A1 (de) * | 2003-05-23 | 2004-12-09 | Basf Ag | Herstellung von Aldehyden, Carbonsäuren und/oder Carbonsäureanhydriden mittels Vanadiumoxid, Titandioxid und Antimonoxid enthaltender Katalysatoren |
DE10334132A1 (de) * | 2003-07-25 | 2005-04-07 | Basf Ag | Silber, Vanadium und ein Promotormetall enthaltendes Multimetalloxid und dessen Verwendung |
DE102004014918A1 (de) | 2004-03-26 | 2005-10-13 | Basf Ag | Katalysator mit einer Silber-Vanadiumoxidphase und einer Promotorphase |
US8097558B2 (en) * | 2004-05-29 | 2012-01-17 | Sud-Chemie Ag | Catalyst and method for producing phthalic anhydride |
US7541489B2 (en) | 2004-06-30 | 2009-06-02 | Sabic Innovative Plastics Ip B.V. | Method of making halophthalic acids and halophthalic anhydrides |
DE102008044890B4 (de) | 2008-08-29 | 2023-09-14 | Stesatec Gmbh | Katalysator für die katalytische Gasphasenoxidation von aromatischen Kohlenwasserstoffen zu Aldehyden, Carbonsäuren und/oder Carbonsäureanhydriden, insbesondere zu Phthalsäureanhydrid, sowie Verfahren zur Herstellung eines solchen Katalysators |
CN102039205B (zh) * | 2009-10-21 | 2012-09-12 | 中国石油化工股份有限公司 | 整体式氮氧化物选择性还原催化剂及其制备方法 |
JP2011121048A (ja) * | 2009-12-09 | 2011-06-23 | Rohm & Haas Co | 固体触媒物質をブレンドし、管状構造物に装填する方法 |
US9573119B2 (en) | 2011-09-16 | 2017-02-21 | Eastman Chemical Company | Process for preparing V—Ti—P catalysts for synthesis of 2,3-unsaturated carboxylic acids |
US8883672B2 (en) * | 2011-09-16 | 2014-11-11 | Eastman Chemical Company | Process for preparing modified V-Ti-P catalysts for synthesis of 2,3-unsaturated carboxylic acids |
US9029289B2 (en) | 2012-07-16 | 2015-05-12 | Basf Se | Catalyst for preparing carboxylic acids and/or carboxylic anhydrides |
WO2014013397A2 (de) * | 2012-07-16 | 2014-01-23 | Basf Se | Katalysator zur herstellung von carbonsäuren und/oder carbonsäureanhydriden |
EP3047904A1 (en) | 2015-01-22 | 2016-07-27 | Basf Se | Catalyst system for oxidation of o-xylene and/or naphthalene to phthalic anhydride |
Family Cites Families (9)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
DE1162348B (de) * | 1961-04-28 | 1964-02-06 | Basf Ag | Verfahren zur Herstellung von Phthalsaeureanhydrid |
DE1642921C3 (de) * | 1965-05-18 | 1978-11-23 | Basf Ag, 6700 Ludwigshafen | Vanadium- und titanhaltiger Trägerkatalysator |
GB1368626A (en) * | 1970-08-26 | 1974-10-02 | Rhone Progil | Catalyst for the oxidation of ortho-xylene to phthalic anhydride |
DE2260615A1 (de) * | 1972-12-12 | 1974-06-20 | Basf Ag | Traegerkatalysator fuer die oxidation von o-xylol oder naphthalin zu phthalsaeureanhydrid |
JPS5143732A (en) * | 1974-10-11 | 1976-04-14 | Nippon Catalytic Chem Ind | Musuifutarusanno seizohoho |
JPS603307B2 (ja) * | 1978-11-29 | 1985-01-26 | 株式会社日本触媒 | 無水フタル酸の製造方法 |
DE2914683A1 (de) * | 1979-04-11 | 1980-10-16 | Basf Ag | Vanadium- und titan- und/oder zirkonhaltiger traegerkatalysator |
JPS591378B2 (ja) * | 1979-12-03 | 1984-01-11 | 株式会社日本触媒 | 無水フタル酸製造用触媒 |
IT1193930B (it) * | 1980-04-02 | 1988-08-31 | Alusuisse Italia Spa | Catalizzatore per la fabbricazione di anidride ftalica |
-
1991
- 1991-03-06 US US07/665,063 patent/US5169820A/en not_active Expired - Lifetime
- 1991-03-08 AU AU72732/91A patent/AU641987B2/en not_active Ceased
- 1991-03-15 DE DE69102169T patent/DE69102169T2/de not_active Expired - Fee Related
- 1991-03-15 AT AT91302270T patent/ATE106278T1/de not_active IP Right Cessation
- 1991-03-15 BR BR919101046A patent/BR9101046A/pt unknown
- 1991-03-15 KR KR1019910004158A patent/KR950008197B1/ko not_active IP Right Cessation
- 1991-03-15 EP EP91302270A patent/EP0447267B1/en not_active Expired - Lifetime
- 1991-03-15 ES ES91302270T patent/ES2054441T3/es not_active Expired - Lifetime
- 1991-03-15 RU SU914895043A patent/RU2047351C1/ru active
- 1991-03-16 CN CN91101762A patent/CN1024092C/zh not_active Expired - Fee Related
Also Published As
Publication number | Publication date |
---|---|
ATE106278T1 (de) | 1994-06-15 |
CN1024092C (zh) | 1994-03-30 |
ES2054441T3 (es) | 1994-08-01 |
DE69102169T2 (de) | 1994-10-20 |
EP0447267A1 (en) | 1991-09-18 |
KR950008197B1 (ko) | 1995-07-26 |
RU2047351C1 (ru) | 1995-11-10 |
EP0447267B1 (en) | 1994-06-01 |
BR9101046A (pt) | 1991-11-05 |
AU641987B2 (en) | 1993-10-07 |
AU7273291A (en) | 1991-09-19 |
DE69102169D1 (de) | 1994-07-07 |
CN1054726A (zh) | 1991-09-25 |
US5169820A (en) | 1992-12-08 |
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