EP1243361A1 - Apparatus for injecting gas into molten metal - Google Patents

Apparatus for injecting gas into molten metal Download PDF

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Publication number
EP1243361A1
EP1243361A1 EP01870054A EP01870054A EP1243361A1 EP 1243361 A1 EP1243361 A1 EP 1243361A1 EP 01870054 A EP01870054 A EP 01870054A EP 01870054 A EP01870054 A EP 01870054A EP 1243361 A1 EP1243361 A1 EP 1243361A1
Authority
EP
European Patent Office
Prior art keywords
porous
gas
molten metal
porous body
refractory
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.)
Withdrawn
Application number
EP01870054A
Other languages
German (de)
English (en)
French (fr)
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
Original Assignee
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 EP01870054A priority Critical patent/EP1243361A1/en
Priority to TW091104685A priority patent/TW584615B/zh
Priority to ARP020100902A priority patent/AR032983A1/es
Priority to DE60205350T priority patent/DE60205350T2/de
Priority to AT02712669T priority patent/ATE301014T1/de
Priority to JP2002573171A priority patent/JP2004531396A/ja
Priority to RU2003127675/02A priority patent/RU2277591C2/ru
Priority to CA002440404A priority patent/CA2440404C/en
Priority to PCT/BE2002/000039 priority patent/WO2002074470A1/en
Priority to ES02712669T priority patent/ES2243701T3/es
Priority to CNB028060903A priority patent/CN1296157C/zh
Priority to HU0303607A priority patent/HU228285B1/hu
Priority to MXPA03008488A priority patent/MXPA03008488A/es
Priority to KR1020037012162A priority patent/KR100874397B1/ko
Priority to BRPI0208100-8A priority patent/BR0208100B1/pt
Priority to EP02712669A priority patent/EP1372888B1/en
Priority to PL364828A priority patent/PL202712B1/pl
Priority to US10/472,642 priority patent/US20040100004A1/en
Publication of EP1243361A1 publication Critical patent/EP1243361A1/en
Priority to ZA200306069A priority patent/ZA200306069B/en
Withdrawn 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 an apparatus for injecting gas into molten metal and to the manufacture of an apparatus 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 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 an apparatus for injecting gas into molten metal through a molten metal-contacting surface comprising
  • an apparatus for injecting gas can be a plug, brick, block, dam, tile, bar, and the like or, more generally, any device capable of injecting gas into a molten metal.
  • the apparatus of the invention can be used to inject any gas (whether reactive or inert) into any molten metal or alloy thereof.
  • the apparatus has at least a molten-metal contacting surface through which the gas is injected.
  • the apparatus 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.
  • 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, magnesia or magnesia spinel, or combinations of any of the above.
  • the apparatus 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 apparatus 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 an apparatus.
  • 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 an apparatus 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 apparatus for injecting gas with lower overall dimensions, achieving the required degree of gas bubbling can be used. This assists in handling of these apparatus during transport and installation in the vessel.
  • 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 an apparatus 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 apparatus 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 an apparatus (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 apparatus 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 apparatus at this temperature for 4 hours and allowing it to cool gently.
  • the following properties have been measured:
  • the apparatus In use the apparatus has injected fine bubbles reliably and constantly.

Landscapes

  • Engineering & Computer Science (AREA)
  • Mechanical Engineering (AREA)
  • Treatment Of Steel In Its Molten State (AREA)
  • Carbon Steel Or Casting Steel Manufacturing (AREA)
  • Furnace Charging Or Discharging (AREA)
  • Casting Support Devices, Ladles, And Melt Control Thereby (AREA)
  • Manufacture And Refinement Of Metals (AREA)
  • Continuous Casting (AREA)
EP01870054A 2001-03-19 2001-03-19 Apparatus for injecting gas into molten metal Withdrawn EP1243361A1 (en)

Priority Applications (19)

Application Number Priority Date Filing Date Title
EP01870054A EP1243361A1 (en) 2001-03-19 2001-03-19 Apparatus for injecting gas into molten metal
TW091104685A TW584615B (en) 2001-03-19 2002-03-13 Plug or brick for injecting gas into molten metal
ARP020100902A AR032983A1 (es) 2001-03-19 2002-03-13 Bloque o ladrillo refractario para inyectar gas en un metal fundido
ES02712669T ES2243701T3 (es) 2001-03-19 2002-03-19 Bloque o ladrillo refractorio para inyectar gas en un metal fundido.
MXPA03008488A MXPA03008488A (es) 2001-03-19 2002-03-19 Bloque o ladrillo refractorio para inyectar gas en un metal fundido.
JP2002573171A JP2004531396A (ja) 2001-03-19 2002-03-19 溶融金属にガスを注入するための耐火性プラグもしくはレンガ
RU2003127675/02A RU2277591C2 (ru) 2001-03-19 2002-03-19 Огнеупорные пробка или блок для нагнетания газа в расплавленный металл
CA002440404A CA2440404C (en) 2001-03-19 2002-03-19 Refractory plug or brick for injecting gas into molten metal
PCT/BE2002/000039 WO2002074470A1 (en) 2001-03-19 2002-03-19 Refractory plug or brick for injecting gas into molten metal
DE60205350T DE60205350T2 (de) 2001-03-19 2002-03-19 Feuerfester baukörper oder stein zum einblasen von gas in geschmolzene metalle
CNB028060903A CN1296157C (zh) 2001-03-19 2002-03-19 用于将气体注入熔融金属的耐火材料塞子或砖及其制造方法
HU0303607A HU228285B1 (hu) 2001-03-19 2002-03-19 Tûzálló dugó vagy tégla gáz injektálásához olvadt fémbe, valamint eljárás annak elõállítására
AT02712669T ATE301014T1 (de) 2001-03-19 2002-03-19 Feuerfester baukörper oder stein zum einblasen von gas in geschmolzene metalle
KR1020037012162A KR100874397B1 (ko) 2001-03-19 2002-03-19 용융된 금속 내에 가스를 주입하는 내화 플러그
BRPI0208100-8A BR0208100B1 (pt) 2001-03-19 2002-03-19 processo para a fabricação de um plugue ou tijolo refratário sólido poroso para revestimento de recipiente para injetar gás em metal em fusão, e, plugue ou tijolo refratário sólido poroso obtido pelo processo.
EP02712669A EP1372888B1 (en) 2001-03-19 2002-03-19 Refractory plug or brick for injecting gas into molten metal
PL364828A PL202712B1 (pl) 2001-03-19 2002-03-19 Lista porowata ogniotrwała zatyczka albo cegła do wyłożenia zbiornika, do wdmuchiwania gazu do roztopionego metalu, oraz sposób jej wytwarzania
US10/472,642 US20040100004A1 (en) 2001-03-19 2002-03-19 Refractory plug or brick for injecting gas into molten metal
ZA200306069A ZA200306069B (en) 2001-03-19 2003-08-06 Refractory plug or brick for injecting gas into molten metal.

Applications Claiming Priority (1)

Application Number Priority Date Filing Date Title
EP01870054A EP1243361A1 (en) 2001-03-19 2001-03-19 Apparatus for injecting gas into molten metal

Publications (1)

Publication Number Publication Date
EP1243361A1 true EP1243361A1 (en) 2002-09-25

Family

ID=8184940

Family Applications (2)

Application Number Title Priority Date Filing Date
EP01870054A Withdrawn EP1243361A1 (en) 2001-03-19 2001-03-19 Apparatus for injecting gas into molten metal
EP02712669A Expired - Lifetime EP1372888B1 (en) 2001-03-19 2002-03-19 Refractory plug or brick for injecting gas into molten metal

Family Applications After (1)

Application Number Title Priority Date Filing Date
EP02712669A Expired - Lifetime EP1372888B1 (en) 2001-03-19 2002-03-19 Refractory plug or brick for injecting gas into molten metal

Country Status (18)

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

Families Citing this family (9)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP1750075A1 (en) 2005-08-05 2007-02-07 Vesuvius Becker & Piscantor Grossalmeroder Schmelztiegelwerke GmbH & Co. KG Crucible for the treatment of molten metal and process for the manufacture thereof
BRPI0617924A2 (pt) * 2005-10-27 2016-08-23 Teijin Pharma Ltd processo de produção, e, composto
DE102005060432A1 (de) * 2005-12-15 2007-06-21 Pa-Ha-Ge Feuerfeste Erzeugnisse Gmbh & Co. Kg Spülkegel
KR200451645Y1 (ko) * 2008-06-27 2011-05-23 김봉려 가열수단이 구비된 보온팩
DE202009014246U1 (de) 2009-10-22 2009-12-24 Knöllinger Keramische Verschleißteile GmbH Gasspülstein
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

Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
GB2096290A (en) * 1981-03-17 1982-10-13 Didier Werke Ag Device for introducing gases into metallurgical vessels
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
JPH03128165A (ja) * 1989-10-11 1991-05-31 Harima Ceramic Co Ltd ポー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

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Publication number Priority date Publication date Assignee Title
DE3833502A1 (de) * 1988-10-01 1990-04-05 Didier Werke Ag Gasspuelstein
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
IN191421B (zh) * 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

Patent Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
GB2096290A (en) * 1981-03-17 1982-10-13 Didier Werke Ag Device for introducing gases into metallurgical vessels
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
JPH03128165A (ja) * 1989-10-11 1991-05-31 Harima Ceramic Co Ltd ポー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

Non-Patent Citations (2)

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Title
PATENT ABSTRACTS OF JAPAN vol. 015, no. 333 (M - 1150) 23 August 1991 (1991-08-23) *
PATENT ABSTRACTS OF JAPAN vol. 1996, no. 03 29 March 1996 (1996-03-29) *

Also Published As

Publication number Publication date
EP1372888B1 (en) 2005-08-03
RU2277591C2 (ru) 2006-06-10
KR20030081527A (ko) 2003-10-17
ATE301014T1 (de) 2005-08-15
BR0208100B1 (pt) 2011-09-06
HUP0303607A3 (en) 2005-05-30
JP2004531396A (ja) 2004-10-14
CA2440404C (en) 2009-06-09
AR032983A1 (es) 2003-12-03
ES2243701T3 (es) 2005-12-01
DE60205350D1 (de) 2005-09-08
TW584615B (en) 2004-04-21
HU228285B1 (hu) 2013-02-28
ZA200306069B (en) 2004-08-06
WO2002074470A1 (en) 2002-09-26
CA2440404A1 (en) 2002-09-26
MXPA03008488A (es) 2003-12-08
BR0208100A (pt) 2004-03-02
US20040100004A1 (en) 2004-05-27
EP1372888A1 (en) 2004-01-02
PL202712B1 (pl) 2009-07-31
PL364828A1 (en) 2004-12-27
RU2003127675A (ru) 2005-04-10
DE60205350T2 (de) 2006-06-01
CN1296157C (zh) 2007-01-24
HUP0303607A2 (hu) 2004-03-01
KR100874397B1 (ko) 2008-12-17
CN1496292A (zh) 2004-05-12

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