EP0022067A1 - Procédé de teinture et de tannage en un seul bain de peaux et de fourrures - Google Patents

Procédé de teinture et de tannage en un seul bain de peaux et de fourrures Download PDF

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Publication number
EP0022067A1
EP0022067A1 EP80810181A EP80810181A EP0022067A1 EP 0022067 A1 EP0022067 A1 EP 0022067A1 EP 80810181 A EP80810181 A EP 80810181A EP 80810181 A EP80810181 A EP 80810181A EP 0022067 A1 EP0022067 A1 EP 0022067A1
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EP
European Patent Office
Prior art keywords
tanning
liquor
carried out
dyes
acid
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.)
Granted
Application number
EP80810181A
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German (de)
English (en)
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EP0022067B1 (fr
Inventor
Klodwald Albiez
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.)
Novartis AG
Original Assignee
Ciba Geigy AG
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.)
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Publication date
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Publication of EP0022067A1 publication Critical patent/EP0022067A1/fr
Application granted granted Critical
Publication of EP0022067B1 publication Critical patent/EP0022067B1/fr
Expired legal-status Critical Current

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Classifications

    • C—CHEMISTRY; METALLURGY
    • C14—SKINS; HIDES; PELTS; LEATHER
    • C14C—CHEMICAL TREATMENT OF HIDES, SKINS OR LEATHER, e.g. TANNING, IMPREGNATING, FINISHING; APPARATUS THEREFOR; COMPOSITIONS FOR TANNING
    • C14C3/00—Tanning; Compositions for tanning
    • D—TEXTILES; PAPER
    • D06—TREATMENT OF TEXTILES OR THE LIKE; LAUNDERING; FLEXIBLE MATERIALS NOT OTHERWISE PROVIDED FOR
    • D06P—DYEING OR PRINTING TEXTILES; DYEING LEATHER, FURS OR SOLID MACROMOLECULAR SUBSTANCES IN ANY FORM
    • D06P3/00—Special processes of dyeing or printing textiles, or dyeing leather, furs, or solid macromolecular substances in any form, classified according to the material treated
    • D06P3/02—Material containing basic nitrogen
    • D06P3/04—Material containing basic nitrogen containing amide groups
    • D06P3/30—Material containing basic nitrogen containing amide groups furs feathers, dead hair, furskins, pelts
    • D06P3/3008—Material containing basic nitrogen containing amide groups furs feathers, dead hair, furskins, pelts using acid dyes

Definitions

  • the present invention relates to a method for single-bath dyeing and tanning of skins or furs.
  • pickled and tanned material When dyeing natural skins and furs, pickled and tanned material is usually used. This means that these three tasks, namely pickling, tanning and dyeing, are carried out in 2 or 3 separate baths, which results in a long treatment time, numerous manipulations and a large amount of personnel. In addition, the coloring can only be carried out at an elevated temperature of at least 50 ° C.
  • the invention has set itself the task of avoiding these disadvantages by specifying a method in which the dyeing is carried out before tanning, with the achievement of uniform and deep shades, and these operations can be carried out in a single bath, thereby reducing the time and Energy and the cost of materials can be significantly reduced.
  • the process according to the invention is single-bath, i.e. performed using only one treatment fleet.
  • the liquor ratio can be chosen within a wide range e.g. 1: 4 to 1:50, preferably 1:10 to 1:40.
  • the temperature at which process steps (a) and (b) are carried out is at least 15 ° C. and as a rule is not higher than 45 ° C. It is preferably in the range from 35 to 40 ° C.
  • the execution of the Process stages (a) and (b) can take a maximum of 24 hours.
  • All natural skins and furs such as e.g. Sheep, goat, beef, veal, foal, rabbit and seal skins, as well as fox, mink fur and other fine furs, including in particular wool sheepskins.
  • These skins and furs are first softened in the usual way by adding a surfactant and then removed on the machine. They are then washed with wetting agents and detergents, if necessary with the addition of alkalis such as e.g. Washed sodium carbonate To largely remove the excess natural fat, dirt and urine residues. The skins or furs are then conveniently wilted or centrifuged.
  • the skins or furs can also be greased with leather greasing agents in the same treatment liquor.
  • Greasing is also carried out at a temperature of 15 to 45 ° C, preferably 30 to 40 ° C.
  • the pH of the greasing can be from 4 to 6.
  • Suitable leather greasing agents are, for example, oils or waxes of natural or synthetic origin, as are generally used for greasing skins and furs. Natural or as waxes Mineral origin as well as mineral or vegetable or animal oils or waxes can be considered. Examples of suitable oils and waxes are castor oil, coconut oil, soybean oil, claw oils, tears, tallow fat, lanolin, cereal germ oil, paraffin oil, white oil, lanolin waxes, paraffin wax, chlorinated and / or sulfated paraffins, fatty acid esters with mono- or polyhydric alcohols such as Oleic acid triglyceride, fatty acid amides or mixtures thereof, optionally also in a mixture with the fatty acids themselves.
  • oils or waxes are preferably used in combination with an anionic, amphoteric or nonionic surfactant or mixtures thereof, which serve as emulsifiers.
  • the anionic surfactants are, for example, acidic, ether groups or ester groups of organic or inorganic acids, preferably sulfated, addition products of allcylene oxides, especially ethylene oxide and / or propylene oxide or also styrene oxide onto aliphatic 'hydrocarbon radicals with a total of at least 8 carbon atoms, organic hydroxyl, carboxyl, Amino and / or amido compounds such as higher fatty alcohols, fatty acids, fatty amines, fatty acid amides or alkylphenols or mixtures of these substances.
  • These addition products can have a degree of alkoxylation of about 2 to 100, in particular 5 to 40, ethoxy and / or propoxy groups.
  • the acidic ethers or esters can be used as free acids or as salts e.g. Alkali metal, alkaline earth metal, ammonium or amine salts are present.
  • amphoteric surfactants are amines or polyamines with 2 or more basic nitrogen atoms, preferably 2 to 5, which have at least one acidic, etherified or esterified polyglycol ether chain and at least one lipophilic substituent and can be partially or completely quaternized.
  • Acid monosulfuric acid esters are among the amphoteric surfactants products of 1 mole of fatty amine or fatty amine mixtures such as tallow fatty amine with 2 to 15 moles of ethylene oxide are particularly preferred.
  • the nonionic surfactants are expediently alkylene oxide addition products of 1 to 50 moles of alkylene oxide, for example ethylene oxide and / or propylene oxide, on 1 mole of an aliphatic monoalcohol with at least 4 carbon atoms, a 3- to 6-valent aliphatic alcohol, one optionally by alkyl or phenyl substituted phenol or a fatty acid having 8 to 22 carbon atoms.
  • nonionic surfactants the addition products of 2 to 15 moles of ethylene oxide with 1 mole of fatty alcohol, fatty acid each with 8 to 18 carbon atoms or alkylphenols with 4 to 12 carbon atoms in the alkyl part are particularly preferred as emulsifiers.
  • the fatliquoring agents used in the process according to the invention are generally used in amounts of 1 to 10 g per liter of liquor.
  • the anionic dyes are, for example, salts of heavy metal-containing or preferably metal-free mono-, dis- or polyazo dyes including the formazan dyes and the anthraquinone, xanthene, nitro, triphenylmethane, naphthoquinoneimine and phthalocyanine dyes.
  • the anionic character of these dyes can be caused by metal sample formation alone and / or preferably by acidic, salt-forming substituents, such as carboxylic acid groups, sulfuric acid and phosphonic acid ester groups, phosphonic acid groups or sulfonic acid groups.
  • These dyes can also have so-called reactive groups in the molecule, which form a covalent bond with the fur to be dyed.
  • the so-called acidic metal-free dyes are preferred.
  • the 1: 1 or 1: 2 metal complex dyes are also of interest.
  • the 1: 1 metal complex agents preferably have one or two sulfonic acid groups. As metal, they contain a heavy metal atom such as Copper, nickel or especially chrome.
  • the 1: 2 metal complex dyes contain a heavy metal atom as the central atom, e.g. a cobalt atom or in particular a chromium atom. Two complex-forming components are connected to the central atom, at least one of which is a dye molecule, but preferably both are dye molecules. The two dye molecules involved in the complex formation can be the same or different from one another.
  • the 1: 2 metal complex dyes can e.g. contain two azomethine molecules, a disazo dye and a monoazo dye, or preferably two monoazo dye molecules.
  • the azo dye molecules can have water solubilizing groups such as e.g. Acid amide, alkylsulfonyl or the above acidic groups. Preference is given to 1: 2 cobalt or 1: 2 chromium complexes of monoazo dyes which have acid amide, alkylsulfonyl or a total of a single sulfonic acid group.
  • Dye mixtures of at least 2 or 3 anionic dyes are particularly preferred for the production of level dichromia or trichromatic dyes.
  • the amount of dyes added to the liquor depends on the desired depth of color. In general, amounts of 0.001 to 10, in particular 0.1 to 5 g, per liter of liquor have proven successful.
  • the dyeing process is preferably carried out in the presence of a leveling agent or dyeing accelerator, which are generally added to the liquor before the dye.
  • the leveling agents can also serve as color accelerators.
  • Non-ionic, cationic or amphoteric surfactants or mixtures thereof can be used as leveling agents or color accelerators.
  • Cationic surfactants have proven to be particularly favorable as leveling agents. proven by attachment from 5 to 15 moles of ethylene oxide are obtained on fatty amines or fatty amine mixtures. These surfactants can also be used in a mixture with nonionic surfactants made from fatty alcohols or alkylphenols and 2 to 15 moles of ethylene oxide.
  • the leveling agent or dyeing accelerator in the dye bath is advantageously 0.5 to 3 g per liter of liquor.
  • the dyebath can additionally contain an organic solvent which is only partially miscible with water and which acts as a color-deepening component.
  • the solvent can advantageously be emulsified with the above-mentioned nonionic surfactants.
  • Preferred organic solvents are those that boil above 80 ° C.
  • Such solvents are e.g. mono- or dihydric aliphatic alcohols with at least 4 carbon atoms, e.g. Butanol, 2-ethylbutanol, 2-ethylhexanol, trimethylhexanol, neopentylglycol; phenoxyethanol, chlorophenoxyethanol; Dialkylene glycol monoalkyl ethers such as e.g. Diethylene glycol monomethyl ether, monoethyl ether, monobutyl ether and monohexyl ether; Acetic acid esters such as e.g.
  • Particularly preferred solvents are butanol, benzyl alcohol, phenoxyethanol and especially tributyl phosphate.
  • the amounts in which these organic solvents are added to the dyebaths alone or as mixtures range from 0.1 g to 80 g, preferably 0.5 to 50 g, per liter of dye liquor.
  • the dyeing baths can contain other conventional additives, such as Contain electrolytes, bactericides, fillers, wetting agents, dispersants, fixatives, diffusion accelerators or defoamers.
  • the fur can be dyed in such a way that the material to be dyed is first treated with the leveling agent or dyeing accelerator for 5 to 15 minutes and then with the dye for 15 to 45 minutes.
  • the dyeing process should take place at a pH of 1 to 4, preferably 2 to 3.
  • the dye liquor is acidified.
  • Mineral acids such as sulfuric acid or phosphoric acid, or preferably lower aliphatic carboxylic acids, such as e.g. Formic, acetic, oxalic, glycolic or lactic acid. Mixtures of these acids can also be used.
  • the fur is also pecked at the same time as dyeing, i.e. prepared for tanning.
  • the coloring and picking of the fur can take a total of 4 to 24 hours, preferably 6 to 12 hours.
  • Suitable tanning agents are, for example, vegetable tanning extracts, synthetic tanning agents, resin tanning agents, aldehydes such as formaldehyde or acetaldehyde or dialdehydes such as glutaraldehyde, dialdehyde starch or mixtures thereof, and acid-reacting auxiliary tanning agents such as condensation products from naphthalenesulfonic acids and formaldehyde, or acid-releasing salts with a tanning effect, such as chromium, aluminum, potassium aluminum or zirconium sulfates, and aluminum silicates. Chromium-containing synthetic tanning agents, preferably based on chromium sulfate, are preferred.
  • the tanning agents can be used in solid or liquid form.
  • the amounts used in which the tanning agents, based on their dry content, are added to the treatment liquors are between 2 to 20 g, preferably 5 to 15 g, per liter of liquor.
  • the tanning should also take place at a pH of 1 to 4.
  • the pH of the liquor for tanning stage (b) is preferably 2.5 to 4.
  • the duration of the tanning can vary depending on the requirements, but is usually 2 to 15 hours.
  • the liquor is usually neutralized with a base.
  • a base e.g. Alkali metal or alkaline earth metal hydroxides, carbonates, bicarbonates, phosphates or borates, especially sodium carbonate, sodium bicarbonate, sodium hydroxide or magnesium hydroxide, as well as aqueous ammonia and lower alkanolamines such as monoethanol, diethanol and triethanolamine.
  • bases can be used in amounts of 2 to 5 g per liter of liquor.
  • the neutralization step can take 1 to 15 hours depending on the addition of the base.
  • the fur material is preferably stored for a further 6 to 48 hours at room temperature.
  • the dyed and tanned fur material is rinsed with water, optionally neutralized with the above-mentioned alkalis and dried and finished in the usual way.
  • the 'process of this invention is obtained by a multistage process, which is carried out in one bath, a uniform dyed skins and furs, which are both extremely soft and supple.
  • the hair side of the fur or fur is mainly dyed, while the leather side is only slightly dyed. This is particularly advantageous for car seat skins, for example.
  • fur dyes such as Light fastness and rub fastness as well as fastness to ironing, tear resistance, fastness to dry cleaning are in no way adversely affected by the single-bath method according to the invention.
  • the percentages are by weight unless otherwise specified.
  • the quantities relate to commercially available, that is to say coupe goods, for the dyes and to the pure substance for the components.
  • the five-digit Color Index numbers (CI) refer to the 3rd edition of the Color Index.
  • Example 1 100 g of wet sheepskin, which has first been soaked, fleshed and washed, are at 38 to 40 ° C in 1 liter of an aqueous liquor containing 50 g of sodium chloride, 0.5 g of 85% formic acid and 8 g of a synthetic Leather greasing agent based on chlorinated and sulfonated paraffin and a mixture of an oxyethylation product of oleic acid reacted with 7 moles of ethylene oxide and the acidic monosulfuric acid ester of the adduct of 14 moles of ethylene oxide with 1 mole of a C 16 -C 18 fatty amine mixture and a pH of 5 , 5, treated for 30 minutes.
  • an aqueous liquor containing 50 g of sodium chloride, 0.5 g of 85% formic acid and 8 g of a synthetic Leather greasing agent based on chlorinated and sulfonated paraffin and a mixture of an oxyethylation product of oleic
  • a cationic leveling agent based on an adduct of 14 moles of ethylene oxide and 1 mole of a C 16 -C 18 fatty acid mixture is added to the liquor and treated for 10 minutes at 38 to 40 ° C.
  • the liquor is then 0.1 g of an acid dye, Acid Orange 3 CI 10385 added and the sheepskin treated at 38 to 40 ° C for a further 30 minutes.
  • the liquor is adjusted to pH 2.8 with 3 g of 85% formic acid and the sheepskin is treated again at 38 to 40 ° C. for 5 hours.
  • 15 g of a chromium-containing synthetic tanning agent are then added to the liquor and the tanning is carried out Fur through at 38 to 40 ° C for 5 hours.
  • the liquor is also slowly with the solution of 3 g of sodium carbonate. added, whereupon the sheepskin is left in the liquor for 12 hours (final pH of the liquor 3.5 to 4).
  • the fur is then stored for 24 hours at room temperature, then rinsed, spun, stretched and dried with warm air. A deep yellow color is obtained on the hair side of the fur with completely open hair.
  • Example 14 100 g of wet sheepskin, which has first been soaked, fleshed and washed, are at 38 ° C. in 1 liter of an aqueous liquor containing 50 g of sodium chloride, 5 g of a synthetic leather greasing agent based on chlorinated and sulfonated paraffin and one with Contains 7 moles of ethylene oxide reacted oxyethylation product of oleic acid and the acidic monosulfuric ester of the adduct of 14 moles of ethylene oxide with 1 mole of a C 10 -C 18 fatty acid mixture and 40 g of benzyl alcohol, treated for 30 minutes.
  • Example 15 -100 g of wet sheepskin, which has first been soaked, fleshed and washed, are at 38 ° C in 1 liter of an aqueous liquor containing 50 g of sodium chloride, 5 g of a synthetic leather greasing agent based on chlorinated and sulfonated paraffin and a Mixture of an oxyethylation product of oleic acid reacted with 7 mol of ethylene oxide and the acidic monosulfuric acid ester of the adduct of 14 mol of ethylene oxide with 1 mol of a C 16 -C 18 fatty acid mixture and 1 g of tributyl phosphate, treated for 30 minutes.
  • a C 16 -C 18 fatty acid mixture and an adduct of 7 moles of ethylene oxide esterified with sulfamic acid and 1 mole of a C 16 -C 18 fatty acid mixture were added to the liquor and treated at 38 ° C. for 10 minutes. After that, the fleet added and the sheepskin treated at 38 ° C for a further 30 minutes. The liquor is then adjusted to pH 2.8 with 3 g of 85% formic acid and the sheepskin is again treated at 38 ° C. for 3 hours. Then 12 g of a chrome-containing synthetic tanning agent are added to the liquor and the tanning of the fur is carried out at 38 ° C. for 12 hours.
  • the solution of 3 g of sodium carbonate is also slowly added to the liquor, whereupon the sheepskin is left in the liquor for 3 hours (final pH of the liquor 3.5 to 4).
  • the fur is then stored for 24 hours at room temperature, neutralized with sodium carbonate solution, then rinsed, spun, stretched and dried with warm air. A deep brown coloring of the hair side of the fur with a completely open hair is obtained.
  • Example 16 100 g of wet sheepskin, which has first been soaked, fleshed and washed, are at 25 ° C in 1 liter of an aqueous liquor containing 50 g of sodium chloride and 5 g of a synthetic leather greasing agent based on chlorinated and sulfated paraffin and a mixture of one 7 moles of ethylene oxide reacted Oxäthyl michreester of the adduct of 14 mol of ethylene oxide with 1 mole of a C 10 - 18 includes -Fettamingemisches, treated for 30 minutes.
  • the liquor is further slowly mixed with the solution of 3 g of sodium carbonate, whereupon the sheepskin is left in the liquor for 12 hours (final pH of the liquor 3.5 to 4).
  • the fur is finally stored for 24 hours at room temperature, neutralized with sodium carbonate solution, then rinsed, spun, stretched and dried with warm air. You get a deep yellow coloring of the hair side of the fur with a completely open hair.

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  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Textile Engineering (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • General Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Coloring (AREA)
EP19800810181 1979-06-06 1980-06-02 Procédé de teinture et de tannage en un seul bain de peaux et de fourrures Expired EP0022067B1 (fr)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
CH5269/79 1979-06-06
CH526979 1979-06-06

Publications (2)

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EP0022067A1 true EP0022067A1 (fr) 1981-01-07
EP0022067B1 EP0022067B1 (fr) 1982-05-05

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EP19800810181 Expired EP0022067B1 (fr) 1979-06-06 1980-06-02 Procédé de teinture et de tannage en un seul bain de peaux et de fourrures

Country Status (6)

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EP (1) EP0022067B1 (fr)
AR (1) AR224007A1 (fr)
BR (1) BR8003523A (fr)
DE (1) DE3060362D1 (fr)
ES (1) ES492122A0 (fr)
NZ (1) NZ193940A (fr)

Cited By (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP0061670A1 (fr) * 1981-03-23 1982-10-06 Ciba-Geigy Ag Procédé de teinture de cuir et de peaux avec des mélanges de colorants
EP0082819A1 (fr) * 1981-12-21 1983-06-29 Ciba-Geigy Ag Utilisation de colorants complexes de cobalt 1:2 pour la teinture du cuir ou des fourrures
US4560386A (en) * 1983-03-21 1985-12-24 Sandoz Ltd. One-bath method for producing tone-in-tone dyeings on sueded wool- or fur-bearing skins
DE19653549A1 (de) * 1996-12-20 1998-06-25 Ciba Geigy Ag Mittel zur Herstellung von Leder

Families Citing this family (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
ES2625320T3 (es) 2013-10-16 2017-07-19 Balenciaga Proceso ecológico de curtido y teñido y producto obtenido

Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US2049547A (en) * 1936-08-04
DE832593C (de) * 1948-03-11 1952-02-25 Ciba A G Verfahren zum Faerben von tierischen Fasern
DE1519507A1 (de) * 1965-02-19 1970-01-15 Felix Schoepp Verfahren zur Uni- und Batikfaerbung,zur Musterung und Veredelung von Pelzfellen,Pelzwaren
US3972675A (en) * 1969-12-03 1976-08-03 Ciba-Geigy Ag Process for dyeing skins and furs
SU614142A1 (ru) * 1976-09-30 1978-07-05 Всесоюзный Научно-Исследовательский Институт Меховой Промышленности Состав дл обработки кожевой ткани меховых шкур

Patent Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US2049547A (en) * 1936-08-04
DE832593C (de) * 1948-03-11 1952-02-25 Ciba A G Verfahren zum Faerben von tierischen Fasern
DE1519507A1 (de) * 1965-02-19 1970-01-15 Felix Schoepp Verfahren zur Uni- und Batikfaerbung,zur Musterung und Veredelung von Pelzfellen,Pelzwaren
US3972675A (en) * 1969-12-03 1976-08-03 Ciba-Geigy Ag Process for dyeing skins and furs
SU614142A1 (ru) * 1976-09-30 1978-07-05 Всесоюзный Научно-Исследовательский Институт Меховой Промышленности Состав дл обработки кожевой ткани меховых шкур

Non-Patent Citations (3)

* Cited by examiner, † Cited by third party
Title
CHEMICAL ABSTRACTS, Band 89, Nr. 14, 2. Oktober 1978, Zusammenfassung Nr. 112461v, Seite 169, Columbus, Ohio, US, & SU - A - 614 142 (AVETISOV et al.) (05-07-1978). *
CHEMISCHES ZENTRABLATT, Band 132, Nr. 52, 27. Dezember 1961, Berlin, DE, R. VRBACKY: "Neue Ansichten uber das Pelzfarben", Seite 18.882, 4. Referat & VEDA VYZKYUM PRUMYSLU KOZEDELNEM Band 5, Seiten 113-122, 1958. *
CHEMISCHES ZENTRALBLATT, Band 125, Nr. 33, 18. August 1954, Berlin, DE, BOGAEWSKI: "Neue Methode zur schnellen Farbung von Pelzen", Seite 7570, 1. Referat & REV. TECHN. IND. CUIR., Band 43, Seiten 70-71, April 1951. *

Cited By (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP0061670A1 (fr) * 1981-03-23 1982-10-06 Ciba-Geigy Ag Procédé de teinture de cuir et de peaux avec des mélanges de colorants
EP0082819A1 (fr) * 1981-12-21 1983-06-29 Ciba-Geigy Ag Utilisation de colorants complexes de cobalt 1:2 pour la teinture du cuir ou des fourrures
US4453942A (en) * 1981-12-21 1984-06-12 Ciba-Geigy Corporation Use of 1:2 cobalt complex dyes for dyeing leather or furs
US4560386A (en) * 1983-03-21 1985-12-24 Sandoz Ltd. One-bath method for producing tone-in-tone dyeings on sueded wool- or fur-bearing skins
DE19653549A1 (de) * 1996-12-20 1998-06-25 Ciba Geigy Ag Mittel zur Herstellung von Leder

Also Published As

Publication number Publication date
DE3060362D1 (en) 1982-06-24
NZ193940A (en) 1982-03-30
ES8104468A1 (es) 1981-04-01
AR224007A1 (es) 1981-10-15
ES492122A0 (es) 1981-04-01
BR8003523A (pt) 1981-01-05
EP0022067B1 (fr) 1982-05-05

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