WO2004074577A1 - Preimpregne - Google Patents

Preimpregne Download PDF

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Publication number
WO2004074577A1
WO2004074577A1 PCT/EP2004/001393 EP2004001393W WO2004074577A1 WO 2004074577 A1 WO2004074577 A1 WO 2004074577A1 EP 2004001393 W EP2004001393 W EP 2004001393W WO 2004074577 A1 WO2004074577 A1 WO 2004074577A1
Authority
WO
WIPO (PCT)
Prior art keywords
resin solution
weight
impregnation
free
polymer dispersion
Prior art date
Application number
PCT/EP2004/001393
Other languages
German (de)
English (en)
Inventor
Arnold Holger
Reinhardt Bernd
Original Assignee
AHLSTROM OSNABRÜCK GmbH
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
Family has litigation
First worldwide family litigation filed litigation Critical https://patents.darts-ip.com/?family=32841851&utm_source=google_patent&utm_medium=platform_link&utm_campaign=public_patent_search&patent=WO2004074577(A1) "Global patent litigation dataset” by Darts-ip is licensed under a Creative Commons Attribution 4.0 International License.
Application filed by AHLSTROM OSNABRÜCK GmbH filed Critical AHLSTROM OSNABRÜCK GmbH
Priority to BRPI0407760-1A priority Critical patent/BRPI0407760B1/pt
Priority to CA2518942A priority patent/CA2518942C/fr
Priority to DE502004001322T priority patent/DE502004001322D1/de
Priority to EP04710840.2A priority patent/EP1518024B2/fr
Priority to ES04710840T priority patent/ES2271845T5/es
Publication of WO2004074577A1 publication Critical patent/WO2004074577A1/fr

Links

Classifications

    • D—TEXTILES; PAPER
    • D21—PAPER-MAKING; PRODUCTION OF CELLULOSE
    • D21H—PULP COMPOSITIONS; PREPARATION THEREOF NOT COVERED BY SUBCLASSES D21C OR D21D; IMPREGNATING OR COATING OF PAPER; TREATMENT OF FINISHED PAPER NOT COVERED BY CLASS B31 OR SUBCLASS D21G; PAPER NOT OTHERWISE PROVIDED FOR
    • D21H27/00—Special paper not otherwise provided for, e.g. made by multi-step processes
    • D21H27/18—Paper- or board-based structures for surface covering
    • D21H27/22—Structures being applied on the surface by special manufacturing processes, e.g. in presses
    • D21H27/26—Structures being applied on the surface by special manufacturing processes, e.g. in presses characterised by the overlay sheet or the top layers of the structures
    • D—TEXTILES; PAPER
    • D21—PAPER-MAKING; PRODUCTION OF CELLULOSE
    • D21H—PULP COMPOSITIONS; PREPARATION THEREOF NOT COVERED BY SUBCLASSES D21C OR D21D; IMPREGNATING OR COATING OF PAPER; TREATMENT OF FINISHED PAPER NOT COVERED BY CLASS B31 OR SUBCLASS D21G; PAPER NOT OTHERWISE PROVIDED FOR
    • D21H17/00—Non-fibrous material added to the pulp, characterised by its constitution; Paper-impregnating material characterised by its constitution
    • D21H17/63—Inorganic compounds
    • D21H17/70—Inorganic compounds forming new compounds in situ, e.g. within the pulp or paper, by chemical reaction with other substances added separately
    • D—TEXTILES; PAPER
    • D21—PAPER-MAKING; PRODUCTION OF CELLULOSE
    • D21H—PULP COMPOSITIONS; PREPARATION THEREOF NOT COVERED BY SUBCLASSES D21C OR D21D; IMPREGNATING OR COATING OF PAPER; TREATMENT OF FINISHED PAPER NOT COVERED BY CLASS B31 OR SUBCLASS D21G; PAPER NOT OTHERWISE PROVIDED FOR
    • D21H25/00—After-treatment of paper not provided for in groups D21H17/00 - D21H23/00
    • D21H25/04—Physical treatment, e.g. heating, irradiating
    • D21H25/06—Physical treatment, e.g. heating, irradiating of impregnated or coated paper

Definitions

  • the invention relates to pre-impregnates, a process for their preparation and decorative coating materials obtainable therefrom.
  • Decorative coating materials so-called decorative papers or decorative foils, are preferably used for surface coating in furniture manufacture and in interior construction, especially for laminate floors. These decorative films are impregnated with synthetic resin and, if necessary, subsequently surface-treated paper webs, which are decoratively printed or unprinted and in a state which can no longer be reactivated under pressure and heat.
  • thermosetting decorative films with a fully impregnated core offline process
  • decorative films based on pre-impregnated materials online process
  • Decorative films based on pre-impregnates are already soaked with a resin mixture within the paper machine, immediately after sheet formation and drying, depending on the mass per unit area of the base paper. After drying and smoothing, usually also within the paper machine, the paper or film must be cross-linked and therefore gap-proof, so that no fiber separation occurs within the decorative film in the subsequent processing steps of the finish coating and lamination on the appropriate carrier.
  • the pre-impregnates for further processing require high opacity and surface quality, good printability in rotogravure printing, good varnishability (high varnish level), good flatness and bondability with chipboard and MDF (medium density fibreboard).
  • the thermally crosslinkable impregnating resins which are usually used for the production of pre-impregnates are water-thinnable, formaldehyde-containing resin solutions based on urea, melamine or phenolic resins. Since their sole use leads to relatively brittle products, these resin solutions are generally used in combination with water-dilutable, thermally crosslinkable polymer dispersions based on acrylic acid, acrylic acid ester, styrene, butadiene, vinyl acetate or acrylonitrile.
  • the resin absorption can be between 5 and 35% by weight, the proportion of resin solutions generally penetrating deeper into the base paper than the proportion of polymer dispersions. The latter accumulate more or less on the top and bottom of the paper and ensure good smoothness and thus printability as well as surface tightness and thus varnishability (varnish level) of the paper.
  • the resin solutions are intended to ensure the good splitting strength and flatness of the pre-impregnate by crosslinking the fiber-resin composite during the further processing processes.
  • the penetration depth of polymer dispersions can be increased by various additives, such as, for example, by water-soluble polymers on the basis of polyvinyl alcohols, gelatin, starches, cellulose derivatives, alginates and their mixtures (EP 0739 435 B1), maleic acid copolymers (EP 0 223 922 A1) or a copolymer of (meth) acrylamide and (meth) acrylic acid (DE 197 28 250 A1 and DE 197 584 79 A1).
  • water-soluble polymers on the basis of polyvinyl alcohols, gelatin, starches, cellulose derivatives, alginates and their mixtures
  • maleic acid copolymers EP 0 223 922 A1
  • a copolymer of (meth) acrylamide and (meth) acrylic acid DE 197 28 250 A1 and DE 197 584 79 A1
  • the pre-impregnates are manufactured using the above-mentioned. Additives completely dispense with the use of classic resin solutions containing formaldehyde. However, these pre-impregnates, which are then free of formaldehyde, are limited in their splitting strength, flatness and printability.
  • chipboard as the last further processing step, does not have any better or even worse internal strengths than known pre-impregnated formaldehyde-free or containing.
  • it up to hot pressing, it has poorer surface tightness and therefore poorer painting (lower paint level) and poorer flatness during lamination (bonding) than previously known formaldehyde-free and containing pre-impregnates.
  • the invention is therefore based on the object of providing partially crosslinked pre-impregnates which largely avoid the disadvantages mentioned at the end of the paper machine and, if possible, have high surface quality, good printability and higher splitting resistance than known pre-impregnates containing or containing formaldehyde, good paintability (high level of lacquer) , good flatness and stickability with common adhesives in the subsequent processing stages and are virtually equivalent in their properties to off-line impregnated papers.
  • the prepreg according to the invention can be obtained by impregnating a base paper with an impregnation combination which contains a thermally curable, formaldehyde-free resin solution and a thermally crosslinkable polymer dispersion.
  • the impregnated base paper is dried and smoothed. The smoothing is expediently carried out within the paper machine used to produce the prepreg.
  • the degree of crosslinking of the pre-impregnate is at least 10% and at most 85%.
  • the impregnated base paper has a residual moisture of 2 to 3% by weight.
  • the degree of crosslinking is determined analogously to the test method described in DE 101 34 302 C1 by punching out an area of 100 cm 2 in a pre-impregnate, weighing it and holding it in water at a temperature of 60 ° C. for 15 minutes, rinsing, in an oven at 130 ° C dried and weighed again.
  • the soluble fraction of the polymer or polymers can be determined from the weight difference and the known application of the impregnating resin or the impregnating combination (for example 12 g / m 2 dry with a 60 g / m 2 pre-impregnate).
  • the degree of crosslinking in% is then 100% soluble in%.
  • the invention also relates to a method for producing thermally partially crosslinked, formaldehyde-free pre-impregnates within the paper machine and their use as decorative coating materials.
  • prepregs are partially impregnated papers with formaldehyde-free resin solutions in combination with polymer dispersions Roger that.
  • the proportion of the impregnation components is 5 to 35% by weight, preferably 10 to 30% by weight, based on the weight of the base paper.
  • the residual moisture of the pre-impregnate is between 1.5 to 3% by weight. At residual moisture levels of more than 3.5% by weight, the pre-impregnate can adhere to machine parts, for example to the smoothing rollers of the paper machine.
  • Suitable formaldehyde-free resin solutions for impregnation are the polymer compositions described in DE 197 35 959 A1, containing
  • a resin can be used to impregnate the base paper which contains the aforementioned components B) and C) but not component A).
  • Such resins are disclosed in DE 197 35 959 A1.
  • the water-dilutable impregnation mixture of the above-mentioned formaldehyde-free resin solutions A) + B) + C) or B) + C) and customarily used polymer dispersions is applied to at least one side of the paper web, then dried to a residual moisture of 2 to 3% by weight and then smoothed.
  • the impregnated base paper is thus partially cross-linked, the degree of cross-linking depending on the mixing ratio of the impregnation combination between at least 10% and max. Is 85%.
  • this is only partially cross-linked pre-impregnate sufficiently flexible.
  • the mixing ratio between formaldehyde-free resin solution (I) and polymer dispersion (II) can be 49:51 to 10:90 (solid), preferably 45:55 to 20:80.
  • Mixing ratios of 35:65 to 30:70 are particularly preferred, since pre-impregnates combined with impregnation combinations. these mixing ratios were produced, are particularly easy to print and are sufficiently flexible.
  • the concentration of the impregnation mixture according to the invention, which contains further additives if required, can be up to 50% by weight.
  • the impregnation combination according to the invention can be applied online to the paper web in an amount between 5 and 35% by weight, preferably between 10 and 30% by weight, based on the basis weight of the base paper. All devices that are usually used within the paper machine can be used as application devices, preferably roller application devices, such as size press or film press.
  • the pre-impregnates according to the invention immediately after the paper machine have better properties than previously known formaldehyde-containing and formaldehyde-free pre-impregnates with regard to printability and surface strength (tesa strength).
  • the partial crosslinking takes place only at the end of the entire process chain of further processing, i.e. hot pressing.
  • These outstanding properties of the pre-impregnate according to the invention are achieved by the combination of resin solutions and polymer dispersions in a specific mixing ratio, in which there is an optimum between the penetrating and film-forming properties of the individual components when impregnating the base paper, and this already within the paper machine, presumably through synergy effects and temperature influence, largely reached its final state.
  • the prepreg according to the invention can be used significantly more universally in the further processing steps and is not subject to any technological restrictions with regard to various process parameters, such as speed, temperature and pressure.
  • the pre-impregnates according to the invention can be produced in such a way that they have a high degree of flexibility, dimensional stability and good barrier properties against water and solvents and can be used in particular as a base material for high-quality special papers, such as printing and advertising media, decorative wall materials, sanding papers, adhesive tapes or floor coverings.
  • pre-impregnate qualities could be achieved if the degree of cross-linking of the pre-impregnate is more than 50%, preferably 70% and more.
  • the base papers to be impregnated according to the invention are those which, inter alia, are described in the patents EP 0223 922 A1, EP 0870 872 A1 and DE 101 34 302 A1.
  • the impregnation, drying and smoothing processes used are also described in detail in the documents mentioned and in the specialist magazine "Wochenblatt für Textilfabrikation" No. 6 (2000), pp. 350 to 355 and known prior art.
  • a base paper was made from 20% pine sulfate pulp and 80% eucalyptus pulp. The freeness was 30 ° SR (Schopper-Riegler). 25% titanium dioxide and 4% formaldehyde-free wet strength agent were used as additives on dry cellulose.
  • This raw paper without size sizing and with a mass per unit area of 48 g / m 2 was impregnated on both sides in a laboratory size press with a formaldehyde-free resin solution of approx. 30% solids content from modified polyacrylic acid and a polyhydric alcohol (Acrodur 950 L from BASF) then dried at different temperatures to a residual moisture of approx. 2% within approx. 18 seconds.
  • the application amount after drying was 10 g / m 2 .
  • Table 1 shows the degrees of crosslinking of the pre-impregnates dried at different temperatures. This is followed by a partial crosslinking of the pre-impregnates up to about 30% under drying conditions customary in the paper machine (up to 110 ° C., drying time approx. 14 seconds at 300 m / min).
  • the base paper from Example 1 was impregnated by means of a laboratory size press with the impregnation mixture according to the invention consisting of a formaldehyde-free resin solution (Acrodur 950 L) and a styrene-acrylate dispersion (Acronal 305 D from BASF) in a ratio of 35:65 (solid) and at temperatures dried from about 110 ° C to a residual moisture of about 2% within about 18 seconds.
  • a formaldehyde-free resin solution Acrodur 950 L
  • a styrene-acrylate dispersion Acronal 305 D from BASF
  • the amount applied was about 12 g / m 2 .
  • the degree of crosslinking of the prepreg according to the invention was approximately 70%. Accordingly, the addition of polymer dispersion to the resin solution significantly increases the degree of crosslinking.
  • Example 3 (comparison)
  • the base paper from Example 1 was processed using a laboratory size press with a commonly used impregnation mixture for classic pre-impregnates made from formaldehyde-free styrene-acrylate dispersion (Acronal 305) and formaldehyde-containing resin solution (Urecoll TS) in a ratio of 70:30 (A) and 90:10 (B) ( calculated) impregnated and then dried analogously to Example 2.
  • the application quantity was approx. 13 g / m 2 in each case.
  • the degree of crosslinking of the classic pre-impregnate was 76% (A) or 84% (B) and is therefore significantly higher than that of pre-impregnates according to the invention with proportions of formaldehyde-free resin solutions according to Examples 1 and 2
  • the formaldehyde-free pre-impregnate according to the invention (Example 2) has significantly better splitting resistance and printability.
  • the paint level remains at a high quality level, while the flatness is somewhat worse.
  • the pre-impregnate according to the invention is characterized by an improved surface tightness and thus significantly higher lacquer level, less color penetration (pinhole test) and better printability and higher flatness.
  • the significantly better properties of the thermally partially crosslinked pre-impregnate according to the invention are caused by the combination of Resin solution and polymer dispersion in a certain range of the mixing ratios and the resulting higher degrees of crosslinking than with the resin solution alone.

Landscapes

  • Reinforced Plastic Materials (AREA)
  • Paper (AREA)
  • Glass Compositions (AREA)
  • Laminated Bodies (AREA)

Abstract

L'invention se rapporte à des préimprégnés productibles par imprégnation d'un papier brut au moyen d'une composition d'imprégnation à réticulation thermique, ainsi qu'à des procédés de production de ces préimprégnés. La composition d'imprégnation contient une solution de résine exempte de formaldéhyde, à réticulation thermique, ainsi qu'une dispersion polymère. Le rapport de mélange entre la solution de résine et la dispersion polymère dans la composition d'imprégnation est compris entre 45:55 et 10:90 (solide-solide). Après une opération de séchage, le préimprégné présente un degré de réticulation minimum de 10 % et maximum de 85 %, ainsi qu'une humidité résiduelle comprise entre 2 et 3 % en poids. Les préimprégnés selon l'invention présentent, dès leur sortie de la machine à papier, de meilleures propriétés en termes d'imprimabilité et de résistance à l'arrachage (cohésion) que les préimprégnés selon l'art antérieur qui contiennent ou non des formaldéhydes. Les préimprégnés selon l'invention présentent en outre une densité superficielle élevée (ce qui facilite l'application de vernis), ainsi qu'une stabilité dimensionnelle/planéité.
PCT/EP2004/001393 2003-02-24 2004-02-13 Preimpregne WO2004074577A1 (fr)

Priority Applications (5)

Application Number Priority Date Filing Date Title
BRPI0407760-1A BRPI0407760B1 (pt) 2003-02-24 2004-02-13 Pré-impregnado e seu processo de produção
CA2518942A CA2518942C (fr) 2003-02-24 2004-02-13 Preimpregne issu de l'impregnation d'un papier support avec un melange de solution resine et de dispersion polymere
DE502004001322T DE502004001322D1 (de) 2003-02-24 2004-02-13 Vorimprägnat
EP04710840.2A EP1518024B2 (fr) 2003-02-24 2004-02-13 Preimpregne
ES04710840T ES2271845T5 (es) 2003-02-24 2004-02-13 Preimpregnado

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
DE10307966A DE10307966C5 (de) 2003-02-24 2003-02-24 Vorimprägnat und Verfahren zu seiner Herstellung
DE10307966.1 2003-02-24

Publications (1)

Publication Number Publication Date
WO2004074577A1 true WO2004074577A1 (fr) 2004-09-02

Family

ID=32841851

Family Applications (1)

Application Number Title Priority Date Filing Date
PCT/EP2004/001393 WO2004074577A1 (fr) 2003-02-24 2004-02-13 Preimpregne

Country Status (7)

Country Link
EP (2) EP1757731A3 (fr)
AT (1) ATE338167T1 (fr)
BR (1) BRPI0407760B1 (fr)
CA (1) CA2518942C (fr)
DE (2) DE10307966C5 (fr)
ES (1) ES2271845T5 (fr)
WO (1) WO2004074577A1 (fr)

Cited By (6)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE102008014558A1 (de) 2008-03-15 2009-09-17 Dracowo Forschungs- Und Entwicklungs Gmbh Polycarbonsäure modifizierte native Epoxide
US7909397B2 (en) 2003-05-15 2011-03-22 Audiovox Corporation In-vehicle docking station for a portable media player
US9321278B2 (en) 2012-08-06 2016-04-26 Unilin, Bvba Method for manufacturing panels having a decorative surface
US10124603B2 (en) 2014-02-06 2018-11-13 Unilin, Bvba Methods for manufacturing panels having a decorative surface
US10471769B2 (en) 2014-01-10 2019-11-12 Unilin, Bvba Method for manufacturing panels having a decorative surface
US11794460B2 (en) 2018-01-04 2023-10-24 Flooring Industries Limited, Sarl Methods for manufacturing panels

Families Citing this family (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP1942141A1 (fr) 2006-12-22 2008-07-09 Rohm and Haas France SAS Composition durcissable
PT2222922T (pt) * 2007-12-17 2017-09-11 Schoeller Technocell Gmbh & Co Kg Impregnado de papel decorativo passível de compressão, que pode ser impresso pelo processo de jato de tinta
DE102013114420A1 (de) 2012-12-23 2014-06-26 Michael Jokiel Imprägnierflotte zur Imprägnierung eines Rohpapieres
US20230313466A1 (en) 2020-06-23 2023-10-05 Sappi Netherlands Services B.V. Barrier paper or board

Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP0739435B1 (fr) * 1993-12-21 1998-10-28 Arjo Wiggins S.A. Feuille de papier impregnee comme revetement decoratif
DE10134302C1 (de) * 2001-07-14 2002-12-12 Technocell Dekor Gmbh & Co Kg Vorimprägnat, Verfahren zu dessen Herstellung sowie daraus erhältliche Dekorimprägnate oder dekorative Beschichtungswerkstoffe
EP1391443A2 (fr) * 2002-08-22 2004-02-25 Armstrong World Industries, Inc. Revêtements sans formaldéhyde et panneau acoustique

Family Cites Families (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE2949306A1 (de) † 1979-12-07 1981-06-11 Letron GmbH, 8750 Aschaffenburg Kunststoff-furnier sowie verfahren zur herstellung eines kunststoff-furnieres
FR2692584B1 (fr) * 1992-06-22 1994-08-26 Buhl Papierfabrick Gmb Geb Nouvelle composition d'imprégnation pour feuilles décoratives pour la fabrication de panneaux stratifiés.
DE19728250C2 (de) * 1997-07-02 2002-01-17 Koehler Decor Gmbh & Co Kg Verfahren zur Herstellung eines Vorimprägnats, das damit erhaltene Vorimprägnat und dessen Verwendung zur Herstellung von Dekorverbundgebilden
DE19735959A1 (de) † 1997-08-19 1999-02-25 Basf Ag Verwendung thermisch härtbarer, wässriger Zusammensetzungen als Bindemittel für Formkörper

Patent Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP0739435B1 (fr) * 1993-12-21 1998-10-28 Arjo Wiggins S.A. Feuille de papier impregnee comme revetement decoratif
DE10134302C1 (de) * 2001-07-14 2002-12-12 Technocell Dekor Gmbh & Co Kg Vorimprägnat, Verfahren zu dessen Herstellung sowie daraus erhältliche Dekorimprägnate oder dekorative Beschichtungswerkstoffe
EP1391443A2 (fr) * 2002-08-22 2004-02-25 Armstrong World Industries, Inc. Revêtements sans formaldéhyde et panneau acoustique

Cited By (18)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US7909397B2 (en) 2003-05-15 2011-03-22 Audiovox Corporation In-vehicle docking station for a portable media player
DE102008014558A1 (de) 2008-03-15 2009-09-17 Dracowo Forschungs- Und Entwicklungs Gmbh Polycarbonsäure modifizierte native Epoxide
US11446938B2 (en) 2012-08-06 2022-09-20 Flooring Industries Limited, Sarl Method for manufacturing panels having a decorative surface
US9321278B2 (en) 2012-08-06 2016-04-26 Unilin, Bvba Method for manufacturing panels having a decorative surface
US11987044B2 (en) 2012-08-06 2024-05-21 Unilin, Bv Method for manufacturing panels having a decorative surface
US10214028B2 (en) 2012-08-06 2019-02-26 Unilin, Bvba Method for manufacturing panels having a decorative surface
US9566823B2 (en) 2012-08-06 2017-02-14 Unilin, Bvba Method for manufacturing panels having a decorative surface
US10549550B2 (en) 2012-08-06 2020-02-04 Unilin, Bvba Method for manufacturing panels having a decorative surface
US10807385B2 (en) 2012-08-06 2020-10-20 Unilin, Bvba Method for manufacturing panels having a decorative surface
US10814648B1 (en) 2012-08-06 2020-10-27 Unilin, Bvba Method for manufacturing panels having a decorative surface
US10906349B2 (en) 2014-01-10 2021-02-02 Unilin Bv Method for manufacturing panels having a decorative surface
US10471769B2 (en) 2014-01-10 2019-11-12 Unilin, Bvba Method for manufacturing panels having a decorative surface
US11465439B2 (en) 2014-01-10 2022-10-11 Flooring Industries Limited, Sarl Method for manufacturing panels having a decorative surface
US11878548B2 (en) 2014-01-10 2024-01-23 Flooring Industries Limited, Sarl Method for manufacturing panels having a decorative surface
US10994555B2 (en) 2014-02-06 2021-05-04 Unilin Bv Methods for manufacturing panels having a decorative surface
US11613133B2 (en) 2014-02-06 2023-03-28 Unilin Bv Methods for manufacturing panels having a decorative surface
US10124603B2 (en) 2014-02-06 2018-11-13 Unilin, Bvba Methods for manufacturing panels having a decorative surface
US11794460B2 (en) 2018-01-04 2023-10-24 Flooring Industries Limited, Sarl Methods for manufacturing panels

Also Published As

Publication number Publication date
CA2518942A1 (fr) 2004-09-02
EP1757731A2 (fr) 2007-02-28
DE10307966C5 (de) 2009-05-28
ES2271845T5 (es) 2013-11-22
CA2518942C (fr) 2014-08-05
BRPI0407760B1 (pt) 2014-04-22
DE10307966A1 (de) 2004-09-09
EP1757731A3 (fr) 2012-12-05
BRPI0407760A (pt) 2006-10-03
EP1518024B1 (fr) 2006-08-30
EP1518024A1 (fr) 2005-03-30
DE502004001322D1 (de) 2006-10-12
EP1518024B2 (fr) 2013-08-07
ATE338167T1 (de) 2006-09-15
DE10307966B4 (de) 2005-08-11
ES2271845T3 (es) 2007-04-16

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