EP1372888B1 - Feuerfester baukörper oder stein zum einblasen von gas in geschmolzene metalle - Google Patents

Feuerfester baukörper oder stein zum einblasen von gas in geschmolzene metalle Download PDF

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Publication number
EP1372888B1
EP1372888B1 EP02712669A EP02712669A EP1372888B1 EP 1372888 B1 EP1372888 B1 EP 1372888B1 EP 02712669 A EP02712669 A EP 02712669A EP 02712669 A EP02712669 A EP 02712669A EP 1372888 B1 EP1372888 B1 EP 1372888B1
Authority
EP
European Patent Office
Prior art keywords
porous
gas
molten metal
plug
brick
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
Application number
EP02712669A
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English (en)
French (fr)
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EP1372888A1 (de
Inventor
Craig Willoughby
Cavan Millward
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Vesuvius Crucible Co
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Vesuvius Crucible Co
Priority date (The priority date 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 date listed.)
Filing date
Publication date
Application filed by Vesuvius Crucible Co filed Critical Vesuvius Crucible Co
Priority to EP02712669A priority Critical patent/EP1372888B1/de
Publication of EP1372888A1 publication Critical patent/EP1372888A1/de
Application granted granted Critical
Publication of EP1372888B1 publication Critical patent/EP1372888B1/de
Anticipated expiration legal-status Critical
Expired - Lifetime legal-status Critical Current

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Classifications

    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B22—CASTING; POWDER METALLURGY
    • B22D—CASTING OF METALS; CASTING OF OTHER SUBSTANCES BY THE SAME PROCESSES OR DEVICES
    • B22D1/00—Treatment of fused masses in the ladle or the supply runners before casting
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B22—CASTING; POWDER METALLURGY
    • B22D—CASTING OF METALS; CASTING OF OTHER SUBSTANCES BY THE SAME PROCESSES OR DEVICES
    • B22D1/00—Treatment of fused masses in the ladle or the supply runners before casting
    • B22D1/002—Treatment with gases
    • B22D1/005—Injection assemblies therefor

Definitions

  • the present invention relates to a refractory plug or brick for vessel lining for injecting gas into molten metal and to the manufacture of a refractory plug or brick for injecting gas into molten metal.
  • Gases are often injected into molten metal in vessels such as ladles, crucibles or tundishes for diverse purposes.
  • a gas may be introduced into the bottom part of a vessel to clear the relatively cool bottom area of solidification products, e.g. to remove them from the vicinity of a bottom pour outlet where the vessel has such an outlet.
  • the use of slow injection of a fine curtain of gas bubbles in the tundish assists in inclusion removal; the inclusions being attracted to the fine gas bubbles and rising upwards through the melt to the surface where they are conventionally captured by the tundish cover powder or flux.
  • Gas may also be introduced for rinsing or to homogenise the melt thermally or compositionally, or to assist in dispersing alloying additions throughout the melt.
  • an inert gas is used but reactive gases may also be employed, e.g. reducing or oxidising gases, when the melt compositions or components thereof needs modifying.
  • gases such as nitrogen, chlorine, freon, sulphur hexafluoride, argon, and the like into molten metal, for example molten aluminium or aluminium alloys, in order to remove undesirable constituents such as hydrogen gas, non-metallic inclusions and alkali metals.
  • the reactive gases added to the molten metal chemically react with the undesired constituents to convert them into a form such as a precipitate, a dross or an insoluble gas compound that can be readily separated from the remainder of the melt.
  • gases or others might also be used for example with steel, copper, iron, magnesium or alloys thereof.
  • the gas be introduced into the molten metal, preferably from the bottom of the recipient, in the form of a very large number of extremely small bubbles.
  • the number of bubbles per unit volume increases.
  • An increase in the number of bubbles and their surface area per unit volume increases the probability of the injected gas being utilised effectively to perform the expected operation.
  • Previous gas injection proposals have included the installation of a solid porous refractory plug or brick in the refractory lining of the vessel, generally on the floor but also in the walls.
  • the plugs or bricks introduce a flow of gas in the form of bubbles.
  • a known technique for introducing gas into molten metal consists of lining a portion of a molten metal-containing vessel (preferably the floor of the vessel) with a porous ceramic body.
  • the gas is introduced into the porous body at a location remote from the metal-contacting surface of the body.
  • the gas follows a number of small, tortuous paths such that a large number of bubbles will be issued into the molten metal.
  • a metal casing that acts as a manifold to introduce gas into the body supports the porous ceramic body.
  • the casing is made of mild steel (for use with inert or slightly reactive gas such as argon or nitrogen) or inconel (for use with highly reactive chlorine or freon).
  • the assembled body/casing is surrounded and supported on all sides except its upper surface by refractory material such as low-cement alumina castable or bricks. When castable is used this can either be cast is situ around the porous body or formed from pre-cast components fixed in place during the hot metal container lining installation. The lining material will "butt" up against the porous body construction.
  • a problem with the foregoing construction is that it is difficult to maintain an effective gas seal between the casing and the body, and between the casing and the support castable/bricks.
  • One difficulty arises in part because the coefficients of thermal expansion of the metal casing and the refractory materials are considerably different; also, the metal casing is subject to attack if chlorine is the gas being used. If a crack should develop (as used herein, the term "crack" refers to any defect in the gas dispersing apparatus that permits undesired gas leakage), gas will leak through the crack, and hereafter frequently will migrate through the next brick and the refractory support to the ambient atmosphere. Gas migration through 50 cm or more or refractory material is possible.
  • the problem is undesirable as the effect of gas leakage upon the flow of gas through the designed gas bubbling surface can be seriously reduced and effectiveness of the bubbling block diminished.
  • gas flow by means of fine gas bubbles will cease and be replaced with uncontrolled direction of gas flow by means of large ineffective gas bubbles.
  • argon is being used the relatively great expense must be considered.
  • the problem is particularly acute in the case of chlorine due to the harmful effects of chlorine upon release into the atmosphere. Regardless of the type of purifying gas being used, it is important that cracks be prevented so that gas leakage will be prevented.
  • a technique would be available for injecting gas into molten metal that would accomplish the objectives of dispersing a large number of exceedingly small bubbles into the molten metal while, at the same time, avoiding cracks in the gas dispersing apparatus that results in gas leakage.
  • any such apparatus could be capable of being manufactured easily, at reasonable expense and having smaller dimensions than the existing apparatus. Further, it would be desirable that any such gas injection apparatus be usable with existing equipment such as a tundish, ladle, melting vessel, and the like, with no modification, or with only minor modification, of the existing equipment.
  • any such gas injection apparatus be compatible with the surrounding refractory materials to prevent any adverse chemical reactions of thermal expansion miss-matches.
  • the invention relates thus to a solid porous refractory plug or brick for vessel lining for injecting gas into molten metal through a molten metal-contacting surface comprising
  • a plug or brick for vessel lining for injecting gas can be a plug, brick, block, dam, tile, bar, and the like.
  • the plug or brick of the invention can be used to inject any gas (whether reactive or inert) into any molten metal or alloy thereof.
  • the plug or brick has at least a molten-metal contacting surface through which the gas is injected.
  • the plug or brick comprises a porous refractory body substantially surrounded by (for example encased by or embedded in) a non-porous body except, of course, at the molten-metal contacting surface. It can be included or form part of the lining of the molten metal vessel.
  • the porous body can be made of any porous refractory material.
  • the nature of the material used is not essential as far as said material has the required porosity.
  • a material having an apparent porosity higher than 20 % is porous.
  • Suitable materials typically comprise alumina, alumina spinel, magnesia or magnesia spinel, or combinations of any of the above.
  • the plug or brick also comprises gas conducting means for conveying the gas from a gas source, to the porous body.
  • the gas conducting means generally comprises a conduit extending through the side wall of the non-porous body.
  • This conduit can be made from metal or a refractory material for example.
  • the conduit can be fixed into place by means of a conventional refractory sealing material (mortar or cement) or it can be pressed within the non-porous body.
  • the gas conducting means comprises a plenum chamber through which the gas contacts a surface of the porous body at least substantially equivalent to the molten metal contacting surface so that the gas is perfectly homogeneously distributed into the porous body and, consequently, will bubble into the molten metal through substantially the whole molten-metal contacting surface.
  • the plug or brick of the present invention is characterised by the fact that the non-porous body is made of refractory material and that the porous and non-porous bodies have been co-pressed. All the above identified requirements are fulfilled with such a plug or brick.
  • non-porous material is not essential as long as it is a refractory material and has the required porosity. Generally, it will be considered that a material having an apparent porosity lower than 20 % is non-porous.
  • the non-porous body and the porous body are preferably constituted of refractory materials with similar coefficients of thermal expansion. This serves to prevent the formation of cracks upon thermal cycling.
  • the granulometry and permeability of the inner porous body can be carefully and consistently controlled to provide an even fine pore structure so that small evenly distributed gas bubbles flow from the molten metal contacting surface of the body.
  • This permeability can be readily adjusted via formulation granulometry changes and a plug or brick according to the invention can be manufactured to suit specific individual customer requirements.
  • This process route is further advantageous in that high magnesia content refractories can be used for the formulations such as magnesia spinel.
  • Such formulations are more compatible with the composition of steel plant tundihs linings which are usually basic (magnesia) based. Chemical and thermal characteristics are therefore very similar.
  • the porous and non-porous refractory bodies have thus a high magnesia content, more than 50 %, preferably more than 80 % and even more preferably more than 90 % by weight of the composition.
  • the co-pressing of the two refractory materials By virtue of the co-pressing of the two refractory materials, the natural low permeability of the non-porous body prevent gas leakage without having to resort to other gas leakage restriction techniques. Another advantage of the co-pressing is that a plug or brick for injecting gas with lower overall dimensions, achieving the required degree of gas bubbling can be used. This assists in handling of these plug or brick during transport and installation in the vessel; in particular in the lining.
  • the co-pressing concept is not restricted to oblong, square, round or oval shapes but can also be used to produce any refractory cross section suitable for co-pressing.
  • a ring co-pressed component can be envisaged which would be located to surround the exit ports of a tundish thereby forming a surrounding stream of gentle rising bubbles though which the hot liquid metal would have to pass prior to entry into the continuous casting moulds.
  • the invention concerns a process for the manufacture of a plug or brick for injecting gas into molten metal. According to the invention, this process comprises the steps of:
  • a delimiter for example made from a thin (but rigid) plastic or metal foil is placed into the mould prior to introducing the refractory material.
  • the delimiter can be shaped as a cylinder (with circular or oval base), or a parallelepiped, without upper and lower surfaces.
  • the refractory material which will form the porous body is then introduced in the central portion formed by the delimiter and the refractory material which will form the non-porous body is introduced between the delimiter and the mould wall.
  • the delimiter is then carefully removed and another amount of the material forming the non-porous body is introduced into the mould to form the surface opposite to the molten metal contacting surface.
  • the step of providing the gas conducting means can be carried out before or after the co-pressing step or both before and after.
  • a plenum chamber is formed by introducing a strip of consumable material into the mould at the junction between the base of the porous body forming material and the adjacent surface of the non-porous body forming material.
  • a hole can be drilled or a conduit placed through the non-porous body after or before co-pressing the materials to connect the porous body (whether or not through the plenum chamber) to an external gas source.
  • the co-pressing step can be carried out according to any known pressing method, for example in an hydraulic press.
  • the heat treating step should be carried out at a temperature sufficient to develop a ceramic bond between the porous and non-porous bodies so that the integrity of the plug or brick and its gas tightness are enhanced.
  • the consumable material (if used) placed to generate the plenum chamber will advantageously be removed during the heat treating step. This consumable material can burn (cardboard, paper) or melt (wax, alloy) at the temperature used.
  • the heat treating step consists in firing the co-pressed material for a temperature comprised between 800 and 1800°C for 2 to 12 hours.
  • FIG. 1 and 2 show cross-sectional views of embodiments of the invention.
  • Both figures show a plug or brick (1) for injecting gas into molten metal through a molten metal-contacting surface (11) comprising a porous refractory body (2) substantially surrounded by a substantially non-porous body (9) except at the molten metal-contacting surface (11).
  • the gas conducting means comprised of a metallic or refractory conduit (4) extending through a wall (6) of the plug or brick and connecting to the plenum chamber (3).
  • the conduit (4) is typically fixed into place by means of a conventional sealing cement or mortar (5).
  • a gradual tapered section (7) is created towards the molten metal-contacting surface (4) during the pressing step as depicted on figure 1.
  • This taper effect is created during the pressing action by the porous body deforming into the non porous medium at the vertical sides of the pressing mould.
  • This tapered shape further protects the porous body (2) by forming a key from major spalling effect.
  • the materials used are the following: (% given by weight): Non-porous body Porous body Silica 0.1 0.13 Alumina 3.3 ( ⁇ 45 ⁇ m) 0.06 Iron oxide 0.2 0.48 Lime 0.4 0.69 Magnesia 96.0 98.5
  • the materials After being introduced into the mould, the materials have been mechanically pressed at a rate to ensure the best possible compaction and integration of the co pressed materials .
  • the heat treating step was carried out by slowly heating the co-pressed material at a rate to avoid thermal fractures/cracking within the pressed body until 1600°C, leaving the plug or brick at this temperature for 4 hours and allowing it to cool gently.
  • the following properties have been measured:
  • the plug or brick In use the plug or brick has injected fine bubbles reliably and constantly.

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  • Engineering & Computer Science (AREA)
  • Mechanical Engineering (AREA)
  • Treatment Of Steel In Its Molten State (AREA)
  • Carbon Steel Or Casting Steel Manufacturing (AREA)
  • Casting Support Devices, Ladles, And Melt Control Thereby (AREA)
  • Furnace Charging Or Discharging (AREA)
  • Manufacture And Refinement Of Metals (AREA)
  • Continuous Casting (AREA)

Claims (10)

  1. Fester poröser Feuerfeststopfen oder -ziegel (1) für eine Behälterauskleidung zum Injizieren von Gas in geschmolzenes Metall durch eine Berührungsfläche (11) zum geschmolzenen Metall, umfassend
    i) einen porösen Feuerfestkörper (2), der im Wesentlichen außer an der Berührungsfläche (11) zum geschmolzenen Metall in einen im Wesentlichen nicht-porösen Körper (9) eingeschlossen ist; und
    ii) eine Gasleiteinrichtung (3, 5) zum Fördern des Gases aus einer Gasquelle zu dem porösen Körper (2),
    dadurch gekennzeichnet, dass der nicht-poröse Körper (11) aus Feuerfestmaterial besteht und dass der poröse und der nicht-poröse Körper (2, 11) gemeinsam gepresst worden sind.
  2. Stopfen oder Ziegel nach Anspruch 1, dadurch gekennzeichnet, dass die Gasleiteinrichtung (3, 5) eine Verteilerkammer (3) umfasst.
  3. Stopfen oder Ziegel nach Anspruch 1 oder 2, dadurch gekennzeichnet, dass der poröse und der nicht-poröse Körper von Feuerfestmaterialien mit ähnlichen Wärmedehnungskoeffizienten gebildet werden.
  4. Stopfen oder Ziegel nach einem der Ansprüche 1 bis 3,
    dadurch gekennzeichnet, dass der poröse und der nicht-poröse Körper von mehr als 50 Gewichts-% Magnesiumoxid, Magnesiumoxid-Spinell, Aluminiumoxid oder Aluminiumoxid-Spinell gebildet werden, vorzugsweise von mehr als 80 Gewichts-%.
  5. Stopfen oder Ziegel nach einem der Ansprüche 1 bis 4,
    dadurch gekennzeichnet, dass der nicht-poröse Körper mehr als 50 Gewichts-%, vorzugsweise mehr als 80 Gewichts-% Magnesiumoxid, Magnesiumoxid-Spinell, Aluminiumoxid oder Aluminiumoxid-Spinell umfasst.
  6. Stopfen oder Ziegel nach einem der Ansprüche 1 bis 5,
    dadurch gekennzeichnet, dass der poröse Körper (2) in Richtung seiner Berührungsfläche zum geschmolzenen Metall hin einen verjüngten Querschnitt (7) aufweist.
  7. Verfahren zur Herstellung eines festen porösen Feuerfeststopfens oder -ziegels für eine Behälterauskleidung zum Injizieren von Gas in geschmolzenes Metall durch eine Berührungsfläche zum geschmolzenen Metall, umfassend die Schritte:
    1) Zuführen von geeigneten Mengen der den porösen und den nicht-porösen Körper bildenden Feuerfestmaterialien in eine Form unter Beachtung der gewünschten Grenzen für diese Körper;
    2) Gleichzeitiges gemeinsames Pressen beider Feuerfestmaterialien;
    3) Bereitstellen einer Gasleiteinrichtung;
    4) Wärmebehandeln der gemeinsam gepressten Materialien.
  8. Verfahren nach Anspruch 7, bei dem die Gasleiteinrichtung eine Verteilerkammer umfasst.
  9. Verfahren nach Anspruch 8, dadurch gekennzeichnet, dass der Schritt (3) eines Bereitstellens der Gasleiteinrichtung einen Schritt eines Einbringens eines Streifens von verzehrbarem Material in die Form an der Stoßstelle zwischen dem porösen und dem nicht-porösen Körper umfasst.
  10. Verfahren nach Anspruch 9, dadurch gekennzeichnet, dass das verzehrbare Material Wachs umfasst.
EP02712669A 2001-03-19 2002-03-19 Feuerfester baukörper oder stein zum einblasen von gas in geschmolzene metalle Expired - Lifetime EP1372888B1 (de)

Priority Applications (1)

Application Number Priority Date Filing Date Title
EP02712669A EP1372888B1 (de) 2001-03-19 2002-03-19 Feuerfester baukörper oder stein zum einblasen von gas in geschmolzene metalle

Applications Claiming Priority (4)

Application Number Priority Date Filing Date Title
EP01870054A EP1243361A1 (de) 2001-03-19 2001-03-19 Vorrichtung zum Einleiten von Gasen in eine Metallschmelze
EP01870054 2001-03-19
PCT/BE2002/000039 WO2002074470A1 (en) 2001-03-19 2002-03-19 Refractory plug or brick for injecting gas into molten metal
EP02712669A EP1372888B1 (de) 2001-03-19 2002-03-19 Feuerfester baukörper oder stein zum einblasen von gas in geschmolzene metalle

Publications (2)

Publication Number Publication Date
EP1372888A1 EP1372888A1 (de) 2004-01-02
EP1372888B1 true EP1372888B1 (de) 2005-08-03

Family

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Family Applications (2)

Application Number Title Priority Date Filing Date
EP01870054A Withdrawn EP1243361A1 (de) 2001-03-19 2001-03-19 Vorrichtung zum Einleiten von Gasen in eine Metallschmelze
EP02712669A Expired - Lifetime EP1372888B1 (de) 2001-03-19 2002-03-19 Feuerfester baukörper oder stein zum einblasen von gas in geschmolzene metalle

Family Applications Before (1)

Application Number Title Priority Date Filing Date
EP01870054A Withdrawn EP1243361A1 (de) 2001-03-19 2001-03-19 Vorrichtung zum Einleiten von Gasen in eine Metallschmelze

Country Status (18)

Country Link
US (1) US20040100004A1 (de)
EP (2) EP1243361A1 (de)
JP (1) JP2004531396A (de)
KR (1) KR100874397B1 (de)
CN (1) CN1296157C (de)
AR (1) AR032983A1 (de)
AT (1) ATE301014T1 (de)
BR (1) BR0208100B1 (de)
CA (1) CA2440404C (de)
DE (1) DE60205350T2 (de)
ES (1) ES2243701T3 (de)
HU (1) HU228285B1 (de)
MX (1) MXPA03008488A (de)
PL (1) PL202712B1 (de)
RU (1) RU2277591C2 (de)
TW (1) TW584615B (de)
WO (1) WO2002074470A1 (de)
ZA (1) ZA200306069B (de)

Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE102005060432A1 (de) * 2005-12-15 2007-06-21 Pa-Ha-Ge Feuerfeste Erzeugnisse Gmbh & Co. Kg Spülkegel
DE202009014246U1 (de) 2009-10-22 2009-12-24 Knöllinger Keramische Verschleißteile GmbH Gasspülstein

Families Citing this family (7)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP1750075A1 (de) 2005-08-05 2007-02-07 Vesuvius Becker & Piscantor Grossalmeroder Schmelztiegelwerke GmbH & Co. KG Tiegel zur Behandlung von flüssigem Metall und Verfahren zu dessen Herstellung
TW200734320A (en) * 2005-10-27 2007-09-16 Teijin Pharma Ltd 3-Hydroxymethylbenzo [b] thiophen derivatives and a process for producing 3-hydroxymethylbenzo [b] thiophen derivatives
KR200451645Y1 (ko) * 2008-06-27 2011-05-23 김봉려 가열수단이 구비된 보온팩
RU2666197C2 (ru) * 2015-08-12 2018-09-06 федеральное государственное бюджетное образовательное учреждение высшего образования "Нижегородский государственный технический университет им. Р.Е. Алексеева" (НГТУ) Способ получения дисперсно-упроченного алюминиевого сплава
US20190113282A1 (en) * 2017-10-12 2019-04-18 Porvair Plc Permeable Bottom Crucible
US11964873B2 (en) * 2019-08-28 2024-04-23 Plassein Technologies Ltd Llc Methods for producing hollow ceramic spheres
US20230313340A1 (en) * 2022-04-05 2023-10-05 Doggone Investment Co. LLC Apparatus and method for production of high purity copper-based alloys

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DE3110204A1 (de) * 1981-03-17 1982-10-14 Didier-Werke Ag, 6200 Wiesbaden Vorrichtung zum einfuehren von gasen in metallurgische gefaesse
US4791978A (en) * 1987-11-25 1988-12-20 Vesuvius Crucible Company Gas permeable stopper rod
US4836508A (en) * 1988-05-03 1989-06-06 Vesuvius Crucible Company Ladle shroud with co-pressed gas permeable ring
DE3833502A1 (de) * 1988-10-01 1990-04-05 Didier Werke Ag Gasspuelstein
JPH03128165A (ja) * 1989-10-11 1991-05-31 Harima Ceramic Co Ltd ポーラスプラグの製造方法
DE4014509A1 (de) * 1990-05-07 1991-11-14 Didier Werke Ag Gasspueler
FR2675064B1 (fr) * 1991-04-09 1995-06-02 Vesuvius France Sa Quenouille comportant une manchette resistant a l'erosion.
GB9212953D0 (en) * 1992-06-18 1992-07-29 Foseco Int Purifying molten metal
CA2073219C (en) * 1992-07-06 1995-12-19 Keizo Aramaki Refractory for gas blowing for molten metal refining vessel
JPH07198267A (ja) * 1993-12-29 1995-08-01 Kawasaki Refract Co Ltd ガス吹込み用ポ−ラスプラグの製造方法
JPH07308759A (ja) * 1994-05-16 1995-11-28 Tokyo Yogyo Co Ltd スライドゲート用プレートれんが
IN191421B (de) * 1994-06-15 2003-11-29 Vesuvius Frnance Sa
JPH08143356A (ja) * 1994-11-17 1996-06-04 Kyushu Refract Co Ltd マグネシア質不焼成れんが
JP2001040413A (ja) * 1999-07-29 2001-02-13 Kurosaki Harima Corp ポーラスプラグ

Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE102005060432A1 (de) * 2005-12-15 2007-06-21 Pa-Ha-Ge Feuerfeste Erzeugnisse Gmbh & Co. Kg Spülkegel
DE202009014246U1 (de) 2009-10-22 2009-12-24 Knöllinger Keramische Verschleißteile GmbH Gasspülstein

Also Published As

Publication number Publication date
JP2004531396A (ja) 2004-10-14
US20040100004A1 (en) 2004-05-27
TW584615B (en) 2004-04-21
WO2002074470A1 (en) 2002-09-26
BR0208100A (pt) 2004-03-02
MXPA03008488A (es) 2003-12-08
CN1296157C (zh) 2007-01-24
RU2277591C2 (ru) 2006-06-10
KR100874397B1 (ko) 2008-12-17
CN1496292A (zh) 2004-05-12
ATE301014T1 (de) 2005-08-15
PL202712B1 (pl) 2009-07-31
EP1243361A1 (de) 2002-09-25
HUP0303607A3 (en) 2005-05-30
HUP0303607A2 (hu) 2004-03-01
ES2243701T3 (es) 2005-12-01
PL364828A1 (en) 2004-12-27
BR0208100B1 (pt) 2011-09-06
DE60205350T2 (de) 2006-06-01
HU228285B1 (hu) 2013-02-28
ZA200306069B (en) 2004-08-06
EP1372888A1 (de) 2004-01-02
RU2003127675A (ru) 2005-04-10
KR20030081527A (ko) 2003-10-17
DE60205350D1 (de) 2005-09-08
CA2440404C (en) 2009-06-09
AR032983A1 (es) 2003-12-03
CA2440404A1 (en) 2002-09-26

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