EP0193107B1 - Etoffe textile liée et procédé pour sa fabrication - Google Patents

Etoffe textile liée et procédé pour sa fabrication Download PDF

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Publication number
EP0193107B1
EP0193107B1 EP86102172A EP86102172A EP0193107B1 EP 0193107 B1 EP0193107 B1 EP 0193107B1 EP 86102172 A EP86102172 A EP 86102172A EP 86102172 A EP86102172 A EP 86102172A EP 0193107 B1 EP0193107 B1 EP 0193107B1
Authority
EP
European Patent Office
Prior art keywords
bonded
binder
weight
fibre fleece
dispersion
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
EP86102172A
Other languages
German (de)
English (en)
Other versions
EP0193107A2 (fr
EP0193107A3 (en
Inventor
Herbert Dr. Dipl.-Chem. Fink
Klaus Dr. Dipl.-Chem. Hübner
Heiner Kniese
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.)
Roehm GmbH Darmstadt
Original Assignee
Roehm GmbH Darmstadt
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 Roehm GmbH Darmstadt filed Critical Roehm GmbH Darmstadt
Publication of EP0193107A2 publication Critical patent/EP0193107A2/fr
Publication of EP0193107A3 publication Critical patent/EP0193107A3/de
Application granted granted Critical
Publication of EP0193107B1 publication Critical patent/EP0193107B1/fr
Anticipated expiration legal-status Critical
Expired - Lifetime legal-status Critical Current

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Classifications

    • D—TEXTILES; PAPER
    • D04—BRAIDING; LACE-MAKING; KNITTING; TRIMMINGS; NON-WOVEN FABRICS
    • D04H—MAKING TEXTILE FABRICS, e.g. FROM FIBRES OR FILAMENTARY MATERIAL; FABRICS MADE BY SUCH PROCESSES OR APPARATUS, e.g. FELTS, NON-WOVEN FABRICS; COTTON-WOOL; WADDING ; NON-WOVEN FABRICS FROM STAPLE FIBRES, FILAMENTS OR YARNS, BONDED WITH AT LEAST ONE WEB-LIKE MATERIAL DURING THEIR CONSOLIDATION
    • D04H1/00—Non-woven fabrics formed wholly or mainly of staple fibres or like relatively short fibres
    • D04H1/40—Non-woven fabrics formed wholly or mainly of staple fibres or like relatively short fibres from fleeces or layers composed of fibres without existing or potential cohesive properties
    • D04H1/42—Non-woven fabrics formed wholly or mainly of staple fibres or like relatively short fibres from fleeces or layers composed of fibres without existing or potential cohesive properties characterised by the use of certain kinds of fibres insofar as this use has no preponderant influence on the consolidation of the fleece
    • D04H1/4326—Condensation or reaction polymers
    • D04H1/435—Polyesters
    • D—TEXTILES; PAPER
    • D04—BRAIDING; LACE-MAKING; KNITTING; TRIMMINGS; NON-WOVEN FABRICS
    • D04H—MAKING TEXTILE FABRICS, e.g. FROM FIBRES OR FILAMENTARY MATERIAL; FABRICS MADE BY SUCH PROCESSES OR APPARATUS, e.g. FELTS, NON-WOVEN FABRICS; COTTON-WOOL; WADDING ; NON-WOVEN FABRICS FROM STAPLE FIBRES, FILAMENTS OR YARNS, BONDED WITH AT LEAST ONE WEB-LIKE MATERIAL DURING THEIR CONSOLIDATION
    • D04H1/00—Non-woven fabrics formed wholly or mainly of staple fibres or like relatively short fibres
    • D04H1/40—Non-woven fabrics formed wholly or mainly of staple fibres or like relatively short fibres from fleeces or layers composed of fibres without existing or potential cohesive properties
    • D04H1/42—Non-woven fabrics formed wholly or mainly of staple fibres or like relatively short fibres from fleeces or layers composed of fibres without existing or potential cohesive properties characterised by the use of certain kinds of fibres insofar as this use has no preponderant influence on the consolidation of the fleece
    • D04H1/425—Cellulose series
    • D04H1/4258—Regenerated cellulose series
    • D—TEXTILES; PAPER
    • D04—BRAIDING; LACE-MAKING; KNITTING; TRIMMINGS; NON-WOVEN FABRICS
    • D04H—MAKING TEXTILE FABRICS, e.g. FROM FIBRES OR FILAMENTARY MATERIAL; FABRICS MADE BY SUCH PROCESSES OR APPARATUS, e.g. FELTS, NON-WOVEN FABRICS; COTTON-WOOL; WADDING ; NON-WOVEN FABRICS FROM STAPLE FIBRES, FILAMENTS OR YARNS, BONDED WITH AT LEAST ONE WEB-LIKE MATERIAL DURING THEIR CONSOLIDATION
    • D04H1/00—Non-woven fabrics formed wholly or mainly of staple fibres or like relatively short fibres
    • D04H1/40—Non-woven fabrics formed wholly or mainly of staple fibres or like relatively short fibres from fleeces or layers composed of fibres without existing or potential cohesive properties
    • D04H1/58—Non-woven fabrics formed wholly or mainly of staple fibres or like relatively short fibres from fleeces or layers composed of fibres without existing or potential cohesive properties by applying, incorporating or activating chemical or thermoplastic bonding agents, e.g. adhesives
    • D04H1/64—Non-woven fabrics formed wholly or mainly of staple fibres or like relatively short fibres from fleeces or layers composed of fibres without existing or potential cohesive properties by applying, incorporating or activating chemical or thermoplastic bonding agents, e.g. adhesives the bonding agent being applied in wet state, e.g. chemical agents in dispersions or solutions
    • D04H1/645—Impregnation followed by a solidification process
    • D—TEXTILES; PAPER
    • D04—BRAIDING; LACE-MAKING; KNITTING; TRIMMINGS; NON-WOVEN FABRICS
    • D04H—MAKING TEXTILE FABRICS, e.g. FROM FIBRES OR FILAMENTARY MATERIAL; FABRICS MADE BY SUCH PROCESSES OR APPARATUS, e.g. FELTS, NON-WOVEN FABRICS; COTTON-WOOL; WADDING ; NON-WOVEN FABRICS FROM STAPLE FIBRES, FILAMENTS OR YARNS, BONDED WITH AT LEAST ONE WEB-LIKE MATERIAL DURING THEIR CONSOLIDATION
    • D04H3/00—Non-woven fabrics formed wholly or mainly of yarns or like filamentary material of substantial length
    • D04H3/013—Regenerated cellulose series
    • D—TEXTILES; PAPER
    • D04—BRAIDING; LACE-MAKING; KNITTING; TRIMMINGS; NON-WOVEN FABRICS
    • D04H—MAKING TEXTILE FABRICS, e.g. FROM FIBRES OR FILAMENTARY MATERIAL; FABRICS MADE BY SUCH PROCESSES OR APPARATUS, e.g. FELTS, NON-WOVEN FABRICS; COTTON-WOOL; WADDING ; NON-WOVEN FABRICS FROM STAPLE FIBRES, FILAMENTS OR YARNS, BONDED WITH AT LEAST ONE WEB-LIKE MATERIAL DURING THEIR CONSOLIDATION
    • D04H3/00—Non-woven fabrics formed wholly or mainly of yarns or like filamentary material of substantial length
    • D04H3/08—Non-woven fabrics formed wholly or mainly of yarns or like filamentary material of substantial length characterised by the method of strengthening or consolidating
    • D04H3/12—Non-woven fabrics formed wholly or mainly of yarns or like filamentary material of substantial length characterised by the method of strengthening or consolidating with filaments or yarns secured together by chemical or thermo-activatable bonding agents, e.g. adhesives, applied or incorporated in liquid or solid form
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y10—TECHNICAL SUBJECTS COVERED BY FORMER USPC
    • Y10S—TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y10S428/00—Stock material or miscellaneous articles
    • Y10S428/913—Material designed to be responsive to temperature, light, moisture
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y10—TECHNICAL SUBJECTS COVERED BY FORMER USPC
    • Y10T—TECHNICAL SUBJECTS COVERED BY FORMER US CLASSIFICATION
    • Y10T442/00—Fabric [woven, knitted, or nonwoven textile or cloth, etc.]
    • Y10T442/20—Coated or impregnated woven, knit, or nonwoven fabric which is not [a] associated with another preformed layer or fiber layer or, [b] with respect to woven and knit, characterized, respectively, by a particular or differential weave or knit, wherein the coating or impregnation is neither a foamed material nor a free metal or alloy layer
    • Y10T442/2861—Coated or impregnated synthetic organic fiber fabric
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y10—TECHNICAL SUBJECTS COVERED BY FORMER USPC
    • Y10T—TECHNICAL SUBJECTS COVERED BY FORMER US CLASSIFICATION
    • Y10T442/00—Fabric [woven, knitted, or nonwoven textile or cloth, etc.]
    • Y10T442/20—Coated or impregnated woven, knit, or nonwoven fabric which is not [a] associated with another preformed layer or fiber layer or, [b] with respect to woven and knit, characterized, respectively, by a particular or differential weave or knit, wherein the coating or impregnation is neither a foamed material nor a free metal or alloy layer
    • Y10T442/2861—Coated or impregnated synthetic organic fiber fabric
    • Y10T442/291—Coated or impregnated polyolefin fiber fabric

Definitions

  • the invention relates to a method for producing bound textile fabrics by applying an acrylic resin dispersion which is free of formaldehyde and formaldehyde-releasing substances.
  • the invention further relates to the textile fabrics produced by the method.
  • Aqueous acyl resin dispersions whose plastic content contained self-crosslinking amide methylol groups have hitherto been used frequently for the production of bound textile fabrics which are notable for high wet strength and for water and wash liquor resistance.
  • binders for textile fabrics which provide sufficient wet strength, water and wash liquor resistance for practical purposes, but do not give off any formaldehyde when heated.
  • EP-A 19 169 describes aqueous dispersions which are suitable as binders for nonwoven fabrics and which contain, as binders, a copolymer of acrylic or methacrylic esters or other monomers and 3 to 10% by weight of units of acrylamidoglycolic acid. It is therefore a binder that does not release formaldehyde when heated. However, since the desired wet strength of the textile fabrics finished with them is not achieved with these binders, small proportions of N-methylolacrylamide are polymerized into the copolymers, thereby increasing the wet strength of the finished fiber structures. however, the risk of formaldehyde release occurs again.
  • EP-A 96 230 describes coating compositions which contain, as self-crosslinking binders, copolymers of acrylic monomers and a crosslinking system composed of methyl acrylamido-glycolic acid methyl ether and hydroxyl, carboxy or amido-functional comonomers. When heated, condensation reactions of the monomer units, the crosslinker system mentioned, occur. It is not known to use such copolymers as binders for textile fabrics.
  • the invention has for its object to produce bonded fabrics with improved wet strength, from whose binder no formaldehyde is released when heated.
  • the bonded fabrics made according to the invention are distinguished from those with conventional formaldehyde-free binders by a significantly increased wet strength. This is important in cases where the bound textile fabric is exposed to mechanical stress during manufacture, further processing or when used in the wet state.
  • a typical application is the production of bonded nonwovens based on synthetic fibers, in particular polyester fibers, which are used for the production of so-called disposable diapers.
  • the bonded non-woven fabrics form the outer cover of the diaper, which envelops a highly absorbent filler. Due to the low water absorption of the synthetic fibers, the outer shell still appears relatively dry when the coated insert has absorbed considerable amounts of liquid. However, it is essential that the outer casing does not tear under mechanical stress and exposes the liquid-saturated insert.
  • the increased wet strength of the textile fabrics bound in the sense of the invention is based on the units of an acrylamidoglycolic acid monomer of the formula as a component of the copolymer contained in the aqueous dispersion.
  • R, R 'and R'' have the meaning given in claim 1.
  • R 'and R'' can be the same alkyl radicals, especially methyl groups.
  • other alkyl radicals with preferably no more than 8 carbon atoms are also suitable, in particular lower alkyl radicals with up to 4 carbon atoms.
  • the acrylic or methacrylic acid alkyl esters forming the main part of the copolymer, or their mixture with styrene, are selected in a manner known per se so that the dynamic freezing temperature T 1max is not more than 60 °, preferably not more than 20 ° C.
  • the copolymer consists of 30 to 60 wt .-% of monomer units that give hard homopolymers, such as methyl, ethyl, propyl, isopropyl methacrylate or styrene, and about 20 to 70% acrylic acid esters of C1 ⁇ 8 alkanols or methacrylic acid esters of C4 ⁇ 8 alkanols.
  • Unsaturated carboxylic acids such as acrylic or methacrylic acid are suitable as further monomer components Amounts of about 1% by weight improve the stability of the dispersion.
  • Crosslinking comonomers such as glycol dimethacrylate, allyl methacrylate, methylene-bis-methacrylamide or butanediol diacrylate, can also improve the strength properties of the binder in small amounts. Too high a proportion of crosslinking agents would interfere with the film formation process and should therefore be avoided.
  • the comonomers which can also be used also include acrylonitrile and methacrylonitrile, vinyl acetate, vinyl chloride, vinylidene chloride and others. Hydroxyesters and amides of acrylic or methacrylic acid are generally not present in the copolymers.
  • the acrylic resin dispersions can be prepared by all common methods of emulsion polymerization. They can contain anionic, cationic or non-ionic emulsifiers or compatible mixtures thereof. They are expediently produced with solids contents of 50 to 70% by weight.
  • the method of the invention is suitable for binding and solidifying textile fabrics of all kinds; these include woven fabrics, knitted fabrics, wadding and in particular non-woven nonwovens.
  • the invention is not restricted to certain types of fibers, but synthetic fibers or fiber mixtures containing synthetic fibers are fundamentally preferred. These mixtures can contain, for example, 70% or more of synthetic fibers.
  • the synthetic fibers considered include fibers made from regenerated cellulose, such as rayon or rayon, and in particular fully synthetic fibers, such as polyester or polypropylene fibers.
  • Preferred textile fabrics are constructed from 70 to 100% by weight of polyester fibers and 0 to 30% by weight of cellulose.
  • the preparation of the dispersion for the consolidation of fiber structures depends on the application process and the requirements placed on the end product.
  • the additives used in these processes like wetting agents. Anti-foaming agents, thermosensitizers. Plasticizers and smoothing agents. Antistatic. Antimicrobials. Dyes, fillers, flame retardants, fragrances, etc. can also be used.
  • the dispersions are diluted with water to a binder content of 10 to 40 percent by weight.
  • the viscosity of the diluted dispersion can range from 10 to 10,000 mPa.s.
  • For the consolidation of wadding for example made of polyester, polyamide or polyacrylonitrile fibers, an approximately 15 to 25% liquor is sprayed on.
  • Compact nonwovens and needle felts can be solidified well by impregnation with 10 to 40% liquors and subsequent squeezing and drying.
  • Light fiber fleeces can also be consolidated by foam impregnation; To do this, foaming agents and foam stabilizers are added to the approximately 10 to 25% dispersion and foamed with air up to a liter weight of 100 to 300 g. The impregnation is expediently carried out on the horizontal foulard.
  • Very light non-woven fabrics can be partially solidified by printing with pastes that contain 20 to 40% binder and are adjusted to a viscosity of 4000 to 8000 mPa.s. Needle felts for high-quality floor and wall coverings are preferably splashed with thickened, possibly foamed liquors. Finally, nonwoven bonding is also possible by brushing.
  • the solidified fiber structures generally contain between 5 and 100%, based on the fiber weight, of binder.
  • the preferred binder content is between 10 and 30% by weight.
  • the fiber structures equipped according to the invention obtain their favorable application properties only by drying at dryer temperatures above 110 ° to about 200 °, preferably in the range between 120 and 160 ° C.
  • a crosslinking agent for example glyoxal, can be added to the dispersion.
  • thermally pre-consolidated polyester fleece with a weight per unit area of approx. 18 g per m2 is impregnated with the plastic dispersion diluted to approx. 25% dry matter, excess dispersion squeezed out with the padding so that a resin coating of approx. 15% is achieved.
  • the damp fleece is dried in the stenter at 140 ° C for 5 minutes.
  • the breaking resistance is determined according to DIN 53 857, Part 2 on dry fleece (F) and on wet fleece (F n ) after 1 hour of water storage in the middle of a tensile testing machine that corresponds to DIN 51 221.
  • a chromatography paper No. 1, Whatman
  • the breaking resistance is determined according to DIN 53 112, sheets 1 and 2.
  • Example 1 illustrates the invention using dispersion A.
  • Example 2 is a comparative test with comparative dispersion B which was not prepared according to the teaching of the invention.
  • Example 3 is a comparison test according to DE-OS 32 02 122.

Landscapes

  • Engineering & Computer Science (AREA)
  • Textile Engineering (AREA)
  • Chemical & Material Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • General Chemical & Material Sciences (AREA)
  • Dispersion Chemistry (AREA)
  • Treatments For Attaching Organic Compounds To Fibrous Goods (AREA)
  • Nonwoven Fabrics (AREA)
  • Macromolecular Compounds Obtained By Forming Nitrogen-Containing Linkages In General (AREA)
  • Materials For Medical Uses (AREA)
  • Manufacture Of Macromolecular Shaped Articles (AREA)

Claims (11)

  1. Procédé de fabrication de produits textiles plats liés par application d'un liant contenant une dispersion aqueuse d'un copolymère de
       80 - 99% en poids d'esters alkyliques d'acide acrylique et/ou méthacrylique à 1-8 atomes de carbone dans le reste alkyle, ou de leurs mélanges avec du styrène,
       1 - 10% en poids d'un monomère acide acrylamidoglycolique,
       0 - 20% en poids d'autres comonomères,
    caractérisé en ce qu'on utilise, comme liant, une dispersion d'un copolymère dont les motifs acide acrylamidoglycolique dérivent de monomères de formule I
    Figure imgb0006
     dans laquelle R est un atome d'hydrogène ou un groupement méthyle, R' est un reste alkyle et R'' est un atome d'hydrogène ou un reste alkyle.
  2. Procédé selon la revendication 1, caractérisé en ce qu'on utilise, comme produit textile plat, une nappe de fibres.
  3. Procédé selon la revendication 2, caractérisé en ce qu'on utilise une nappe de fibres qui est constituée en totalité ou en majorité par des fibres synthétiques.
  4. Procédé selon la revendication 3, caractérisé en ce qu'on utilise une nappe de fibres dont la part de fibres synthétiques est faite, au moins en partie, de fibres de polyester.
  5. Procédé selon l'une quelconque des revendications 1 à 4, caractérisé en ce que dans les motifs acide acrylamidoglycolique de formule I, R'' est un reste alkyle.
  6. Produit textile plat lié, contenant, en tant que liant, un copolymère de
       80 - 99% en poids d'esters alkyliques d'acide acrylique et/ou méthacrylique à 1-8 atomes de carbone dans le reste alkyle, ou de leurs mélanges avec du styrène,
       1 - 10% en poids d'un monomère acide acrylamidoglycolique,
       0 - 20% en poids d'autres comonomères.
  7. Nappe de fibres liée selon la revendication 6, caractérisée en ce que dans les motifs acide acrylamidoglycolique de formule I, R'' est un reste alkyle.
  8. Produit textile plat lié selon la revendication 6 ou 7, caractérisé en ce qu'il s'agit d'une nappe de fibres non tissée et liée.
  9. Nappe de fibres liée selon la revendication 8, caractérisée en ce que la partie fibres est faite en majorité ou entièrement de fibres synthétiques.
  10. Nappe de fibres liée selon la revendication 9, caractérisée en ce que les fibres synthétiques sont constituées en majorité ou en totalité de fibres de polyester.
  11. Nappe de fibres liée selon la revendication 9 ou 10, caractérisée en ce qu elle contient de 10 à 40% en poids de liant.
EP86102172A 1985-02-28 1986-02-19 Etoffe textile liée et procédé pour sa fabrication Expired - Lifetime EP0193107B1 (fr)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
DE19853507154 DE3507154A1 (de) 1985-02-28 1985-02-28 Gebundenes textiles flaechengebilde und verfahren zu seiner herstellung
DE3507154 1985-02-28

Publications (3)

Publication Number Publication Date
EP0193107A2 EP0193107A2 (fr) 1986-09-03
EP0193107A3 EP0193107A3 (en) 1989-07-19
EP0193107B1 true EP0193107B1 (fr) 1992-04-22

Family

ID=6263831

Family Applications (1)

Application Number Title Priority Date Filing Date
EP86102172A Expired - Lifetime EP0193107B1 (fr) 1985-02-28 1986-02-19 Etoffe textile liée et procédé pour sa fabrication

Country Status (7)

Country Link
US (1) US4689264A (fr)
EP (1) EP0193107B1 (fr)
JP (1) JPS61201061A (fr)
DE (2) DE3507154A1 (fr)
DK (1) DK165844C (fr)
FI (1) FI84188C (fr)
NO (1) NO164181C (fr)

Families Citing this family (6)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE3734752A1 (de) * 1987-10-14 1989-05-03 Basf Ag Verfahren zur herstellung von waessrigen (meth)acrylsaeureester-copolymer-dispersionen in zwei stufen und deren verwendung als impraegnier-, ueberzugs- und bindemittel fuer flaechige fasergebilde
US5369204A (en) * 1991-11-01 1994-11-29 Cytec Technology Corp. Low molecular weight acrylamidoglycolate crosslinker and process
US5486210A (en) 1992-01-30 1996-01-23 Reeves Brothers, Inc. Air bag fabric containing graft polymer thereon
US5407728A (en) 1992-01-30 1995-04-18 Reeves Brothers, Inc. Fabric containing graft polymer thereon
ES2103583T3 (es) * 1993-06-02 1997-09-16 Minnesota Mining & Mfg Articulos no tejidos y metodos para producirlos.
DE4344149A1 (de) * 1993-12-23 1995-06-29 Basf Ag Formaldehydfreie wäßrige Kunstharzdispersionen

Family Cites Families (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE2920377A1 (de) * 1979-05-19 1980-12-04 Basf Ag Binde-, impraegnier- und ueberzugsmittel auf basis einer waessrigen dispersion eines amidgruppenhaltigen copolymerisats
CA1135712A (fr) * 1979-05-29 1982-11-16 Peter J. Schirmann Monomeres et polymeres d'ester actives
DE3202122A1 (de) * 1982-01-23 1983-07-28 Röhm GmbH, 6100 Darmstadt Verfahen zum verfestigen von fasergebilden mittels waessriger kunststoffdispersionen
US4454301A (en) * 1982-06-07 1984-06-12 American Cyanamid Company Crosslinking coating compositions

Also Published As

Publication number Publication date
NO855106L (no) 1986-08-29
JPS61201061A (ja) 1986-09-05
NO164181B (no) 1990-05-28
EP0193107A2 (fr) 1986-09-03
FI860802A0 (fi) 1986-02-25
DK87686D0 (da) 1986-02-25
EP0193107A3 (en) 1989-07-19
FI84188C (fi) 1991-10-25
FI860802A (fi) 1986-08-29
NO164181C (no) 1990-09-05
DE3507154C2 (fr) 1993-01-21
US4689264A (en) 1987-08-25
DK87686A (da) 1986-08-29
DE3684937D1 (de) 1992-05-27
FI84188B (fi) 1991-07-15
DK165844C (da) 1993-06-21
DE3507154A1 (de) 1986-08-28
DK165844B (da) 1993-01-25

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