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WO1992022609A1 - Sealants and adhesives based on silane-modified prepolymers - Google Patents

Sealants and adhesives based on silane-modified prepolymers Download PDF

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Publication number
WO1992022609A1
WO1992022609A1 PCT/EP1992/001194 EP9201194W WO9222609A1 WO 1992022609 A1 WO1992022609 A1 WO 1992022609A1 EP 9201194 W EP9201194 W EP 9201194W WO 9222609 A1 WO9222609 A1 WO 9222609A1
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Prior art keywords
compositions according
fluorosurfactants
prepolymers
silane
compositions
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.)
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Application number
PCT/EP1992/001194
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German (de)
French (fr)
Inventor
Gabriele Bride
Manfred Proebster
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Henkel Teroson GmbH
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Henkel Teroson GmbH
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Publication of WO1992022609A1 publication Critical patent/WO1992022609A1/en
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Classifications

    • CCHEMISTRY; METALLURGY
    • C09DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09KMATERIALS FOR MISCELLANEOUS APPLICATIONS, NOT PROVIDED FOR ELSEWHERE
    • C09K3/00Materials not provided for elsewhere
    • C09K3/10Materials in mouldable or extrudable form for sealing or packing joints or covers
    • CCHEMISTRY; METALLURGY
    • C08ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08GMACROMOLECULAR COMPOUNDS OBTAINED OTHERWISE THAN BY REACTIONS ONLY INVOLVING UNSATURATED CARBON-TO-CARBON BONDS
    • C08G65/00Macromolecular compounds obtained by reactions forming an ether link in the main chain of the macromolecule
    • C08G65/02Macromolecular compounds obtained by reactions forming an ether link in the main chain of the macromolecule from cyclic ethers by opening of the heterocyclic ring
    • C08G65/32Polymers modified by chemical after-treatment
    • C08G65/329Polymers modified by chemical after-treatment with organic compounds
    • C08G65/336Polymers modified by chemical after-treatment with organic compounds containing silicon
    • CCHEMISTRY; METALLURGY
    • C08ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08KUse of inorganic or non-macromolecular organic substances as compounding ingredients
    • C08K5/00Use of organic ingredients
    • C08K5/02Halogenated hydrocarbons
    • CCHEMISTRY; METALLURGY
    • C08ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08LCOMPOSITIONS OF MACROMOLECULAR COMPOUNDS
    • C08L101/00Compositions of unspecified macromolecular compounds
    • C08L101/02Compositions of unspecified macromolecular compounds characterised by the presence of specified groups, e.g. terminal or pendant functional groups
    • C08L101/10Compositions of unspecified macromolecular compounds characterised by the presence of specified groups, e.g. terminal or pendant functional groups containing hydrolysable silane groups
    • CCHEMISTRY; METALLURGY
    • C09DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09KMATERIALS FOR MISCELLANEOUS APPLICATIONS, NOT PROVIDED FOR ELSEWHERE
    • C09K2200/00Chemical nature of materials in mouldable or extrudable form for sealing or packing joints or covers
    • C09K2200/02Inorganic compounds
    • C09K2200/0239Oxides, hydroxides, carbonates
    • CCHEMISTRY; METALLURGY
    • C09DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09KMATERIALS FOR MISCELLANEOUS APPLICATIONS, NOT PROVIDED FOR ELSEWHERE
    • C09K2200/00Chemical nature of materials in mouldable or extrudable form for sealing or packing joints or covers
    • C09K2200/04Non-macromolecular organic compounds
    • C09K2200/0411Halogen-containing compounds
    • CCHEMISTRY; METALLURGY
    • C09DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09KMATERIALS FOR MISCELLANEOUS APPLICATIONS, NOT PROVIDED FOR ELSEWHERE
    • C09K2200/00Chemical nature of materials in mouldable or extrudable form for sealing or packing joints or covers
    • C09K2200/04Non-macromolecular organic compounds
    • C09K2200/0447Fats, fatty oils, higher fatty acids or derivatives thereof
    • CCHEMISTRY; METALLURGY
    • C09DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09KMATERIALS FOR MISCELLANEOUS APPLICATIONS, NOT PROVIDED FOR ELSEWHERE
    • C09K2200/00Chemical nature of materials in mouldable or extrudable form for sealing or packing joints or covers
    • C09K2200/06Macromolecular organic compounds, e.g. prepolymers
    • C09K2200/0615Macromolecular organic compounds, e.g. prepolymers obtained by reactions only involving carbon-to-carbon unsaturated bonds
    • C09K2200/0635Halogen-containing polymers, e.g. PVC
    • CCHEMISTRY; METALLURGY
    • C09DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09KMATERIALS FOR MISCELLANEOUS APPLICATIONS, NOT PROVIDED FOR ELSEWHERE
    • C09K2200/00Chemical nature of materials in mouldable or extrudable form for sealing or packing joints or covers
    • C09K2200/06Macromolecular organic compounds, e.g. prepolymers
    • C09K2200/068Containing also other elements than carbon, oxygen or nitrogen in the polymer main chain
    • C09K2200/0685Containing silicon

Definitions

  • the invention relates to compositions based on branched or unbranched prepolymers modified with silane at the chain ends, a process for their preparation and their use.
  • Adhesives and sealants reacting when moisture enters into elastic masses are known. They usually consist of a moisture-reactive prepolymer, plasticizers, fillers and additives as well as a catalyst system.
  • US Pat. No. 3,971,751 describes compounds which are moisture-reactive and which carry silicon atoms with at least one hydrolyzable radical at the chain ends, with the hydrolyzable group (s) being, for example, alkoxy, aminoxy, acid amide or ketoximato groups own.
  • the dimethoxymethylsilyl group is mentioned as the preferred silyl end group.
  • EP 0 326 862 A further method for reducing the surface tack is described in EP 0 326 862, in which fluorine compounds containing silicon groups are used to reduce the tack.
  • fluorine compounds containing silicon groups are used to reduce the tack.
  • these compounds have the disadvantage that they are sensitive to hydrolysis and, moreover, can intervene in the polymer system as chain terminators, the more the more additive is added, the more so.
  • compositions of different wettable silicone prepolymers based on siloxanes which contain ethoxylated, nonionic surfactants or fluorosurfactants. These surfactants serve to make the silicone crosslinked later hydrophilic.
  • a disadvantage of the compositions containing these fluorosurfactants 5 is, however, that the fluorosurfactants prevent or at least considerably complicate the overpainting of the crosslinked silicone.
  • the object of the invention is to avoid the disadvantages mentioned and to provide compositions based on silane-modified prepolymers which lead to a crosslinked polymer, the surface tack of which is considerably reduced, but which is nevertheless overlaid with aqueous dispersions - can be. 15
  • the invention is also based on the object of making it possible to reduce the surface tack while maintaining good paintability by means of an easy-to-handle and commercially available additive.
  • compositions which contain branched or unbranched prepolymers and fluorosurfactants which are silane-modified at the chain ends.
  • R and R ' are used, wherein R and R 'are alkyl, alkoxy, aminoxy, acid amide or ketoximato groups, n is a number from 1 to 35,500, in particular from 100 to 300 and a is a number from 0 to 2, where at least a hydrolyzable group is bonded directly to the Si atom.
  • R is a branched or unbranched CC 10 alkyl group, particularly preferably a Cx-Cs-alkyl group and in particular a methyl group and R 'is an alkoxy group, a ketoximato group, an aminoxy group, particularly preferably an alkoxy group with the structure OR ", where R "is a C ! -C 10 - alkyl group, particularly preferably a Ci-Cs alkyl group and in particular a methyl group.
  • inert, solid or liquid, saturated fluorine compounds which are also known as fluorosurfactants, are used as additives with respect to the silane-modified prepolymer.
  • Aliphatic fluorosurfactants are preferably used. In their chemical structure they correspond to fluorinated alkyl (poly) alkoxylates, fluorinated alkyl (poly) sulfonamides or mixtures thereof. Compounds of this type are sold under the names Fluorad ® or Dynamar ® by 3M for example. If appropriate, these fluorosurfactants can be mixed with further fluorine compounds.
  • the compositions according to the invention contain 0.01 to 10% by weight, in particular 0.05 to 5% by weight, of fluorine compounds, based on the weight of the compositions.
  • compositions according to the invention can contain one or more unbranched or branched silane-modified prepolymer components and further optionally other polymers or prepolymers.
  • other additives such as plasticizers, fillers, silanes, antioxidants, dyes or catalysts can be present in the compositions.
  • compositions according to the invention are prepared by mixing the prepolymers with the fluorine compounds and, if appropriate, with the addition of further additives specified above.
  • the fluorine compounds are preferably added at the beginning of the preparation of the mixture. If solid fluorine compounds are used, it may be advisable to pre-dissolve them in a plasticizer or a solvent. paste to ensure a quick and homogeneous distribution in the prepolymer.
  • the fluorine compounds in the compositions according to the invention do not impair the ability to be painted over. Due to the lack of siloxane oligomers, the sealing compounds according to the invention are also absolutely "free from discoloration".
  • Recipe A is a comparative example that contains no fluorosurfactant.
  • formulation C contains, in addition to 30% of the silane-modified prepolymer, 5% of polyvinyl chloride. The figures are in% by weight.
  • compositions A, B and C were applied to glass or polyethylene plates or lacquered wood in order to test adhesion, Shore A hardness, through-hardening speed and surface tack. The results are summarized in Table 2.
  • the fluorosurfactants according to the invention can of course also be used in multi-component, preferably in two-component systems.
  • the latter is understood to mean systems in which the hardening is accomplished not by diffusing air humidity but by mixing two or more components.

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  • Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Health & Medical Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Medicinal Chemistry (AREA)
  • Polymers & Plastics (AREA)
  • Engineering & Computer Science (AREA)
  • Materials Engineering (AREA)
  • General Chemical & Material Sciences (AREA)
  • Compositions Of Macromolecular Compounds (AREA)
  • Sealing Material Composition (AREA)

Abstract

The invention concerns compositions containing branched or unbranched prepolymers and fluorosurfactants silane-modified at the chain ends. The compositions have low surface tackiness and can be easily painted over after curing. In addition, the invention concerns a method of manufacturing the compositions, and their use as sealants and adhesives.

Description

Dicht- und Klebstoffe auf Basis silanmodifizierter Präpolymere Sealants and adhesives based on silane-modified prepolymers

Die Erfindung betrifft Zusammensetzungen auf Basis verzweigter oder unverzweigter an den Kettenenden silanmodifizierter Präpo¬ lymere, ein Verfahren zu deren Herstellung und deren Verwendung.The invention relates to compositions based on branched or unbranched prepolymers modified with silane at the chain ends, a process for their preparation and their use.

Bei Zutritt von Feuchtigkeit zu elastischen Massen reagierende Kleb- und Dichtstoffe sind bekannt. Sie bestehen in der Regel aus einem feuchtigkeitsreaktiven Präpolymer, Weichmacher, Füll- und Zusatzstoffen sowie einem Katalysatorsystem. Als feuchtig¬ keitsreaktive Präpolymere wurden in der US-PS 3 971 751 Verbin¬ dungen beschrieben, die an den Kettenenden Siliciumatome mit mindestens einem hydrolysierbaren Rest tragen, wobei sich als hydrolisierbare Gruppe(n) z.B. Alkoxy-, Aminoxy-, Säureamid- oder Ketoximatogruppen eignen. Als bevorzugte Silylendgruppe wird die Dimethoxymethylsilylgruppe genannt. In Abhängigkeit von den bei der Synthese der silanmodifizierten Präpolymere verwen¬ deten Rohstoffe lassen sich auch höherwertige (z.B. dreiwertige) Präpolymere mit Silylendgruppen herstellen. Bei der Formulierung von Kleb-, insbesondere aber von weichen Dichtstoffen auf Basis der obengenannten silan odifizierten Präpolymere ergeben sich Produkte, die auch nach vollständiger Durchhärtung noch eine erhebliche Oberflächenklebrigkeit, auch "Tack" genannt, aufwei- sen. Dies ist für viele Anwendungen von so großem Nachteil, daß oftmals zu anderen Dichtstoffen gegriffen werden muß, die zwar weniger Tack aufweisen, aber anderweitige Nachteile zeigen. Beispielsweise ist bei der Einglasung von Fenstern eine Grund- Voraussetzung, daß der deutlich sichtbare Dichtstoff in der Fuge zwischen Fensterglas und -rahmen eine glatte und staubfreie Oberfläche aufweist, die gegebenenfalls mit üblichen Mitteln leicht zu reinigen sein muß. Weist ein Dichtstoff nach der Bil¬ dung einer Oberflächenhaut jedoch noch einen erheblichen Rest- Tack auf, d.h. deutlich spürbare Oberflächenklebrigkeit, kann sich beispielsweise Staub auf dem Dichtstoff absetzen. Der an dem Dichtstoff haftende Staub ist dann mit einfachen Mitteln nicht mehr entfernbar.Adhesives and sealants reacting when moisture enters into elastic masses are known. They usually consist of a moisture-reactive prepolymer, plasticizers, fillers and additives as well as a catalyst system. US Pat. No. 3,971,751 describes compounds which are moisture-reactive and which carry silicon atoms with at least one hydrolyzable radical at the chain ends, with the hydrolyzable group (s) being, for example, alkoxy, aminoxy, acid amide or ketoximato groups own. The dimethoxymethylsilyl group is mentioned as the preferred silyl end group. Depending on the raw materials used in the synthesis of the silane-modified prepolymers, higher-quality (eg trivalent) prepolymers with silyl end groups can also be produced. When formulating adhesives, but especially soft sealants, based on the above-mentioned silane-modified prepolymers, products are obtained which, even after they have completely hardened, still have considerable surface tack, also called "tack". sen. For many applications this is such a disadvantage that it is often necessary to resort to other sealants which have less tack but show other disadvantages. For example, when windows are glazed in, a basic prerequisite is that the clearly visible sealant in the joint between the window glass and frame has a smooth and dust-free surface, which may have to be easy to clean with conventional means. However, if a sealant has a considerable residual tack after the formation of a surface skin, ie clearly noticeable surface stickiness, dust can, for example, settle on the sealant. The dust adhering to the sealant can then no longer be removed with simple means.

In der Literatur wurde dieser Nachteil der unter Verwendung von silanmodifiziertenPräpolymeren (SMP-Präpolymeren) hergestellten Dichtstoffe bereits vor längerem beschrieben. Es sind daher Ver¬ suche unternommen worden, diesen Mangel zu beheben. In der EP 0 327 896 wird z.B. beschrieben, daß durch Zugabe von luftoxi- dierbaren Verbindungen wie Leinöl oder Polybutadienöl eine kleb¬ freie Haut erzielt werden kann. Nachteilig ist hierbei jedoch, daß der Vorgang der "Lufttrocknung", d.h. der oxidativen Ver¬ netzung des Additivs, einen langen Zeitraum in Anspruch nimmt, in der Regel mehrere Tage bis Wochen. Während dieser Zeit kann sich aber, bedingt durch den noch vorhandenen Tack, Staub auf dem Dichtstoff absetzen.This disadvantage of the sealants produced using silane-modified prepolymers (SMP prepolymers) has been described for some time in the literature. Attempts have therefore been made to remedy this deficiency. EP 0 327 896 e.g. described that a tack-free skin can be achieved by adding air-oxidizable compounds such as linseed oil or polybutadiene oil. The disadvantage here, however, is that the "air drying" process, i.e. the oxidative crosslinking of the additive takes a long time, usually several days to weeks. During this time, due to the tack still present, dust can settle on the sealant.

Ein weiteres Verfahren zur Verminderung der Oberflächenklebrig¬ keit wird in der EP 0 326 862 beschrieben, bei dem zur Tackver- minderung siliciumgruppenhaltige Fluorverbindungen eingesetzt werden. Diese Verbindungen weisen neben ihrer schweren Zugäng¬ lichkeit den Nachteil auf, daß sie hydrolyseempfindlich sind und zudem als Kettenabbrecher in das Polymersystem eingreifen kön¬ nen, dies um so stärker, je mehr Additiv zugesetzt wird.A further method for reducing the surface tack is described in EP 0 326 862, in which fluorine compounds containing silicon groups are used to reduce the tack. In addition to being difficult to access, these compounds have the disadvantage that they are sensitive to hydrolysis and, moreover, can intervene in the polymer system as chain terminators, the more the more additive is added, the more so.

Ferner sind in der US-PS 4 657 959 Zusammensetzungen aus ver- netzbaren Silikon-Präpolymeren auf Basis von Siloxanen beschrie¬ ben, die ethoxylierte, nichtionische Tenside oder Fluortenside enthalten. Diese Tenside dienen dazu, das später vernetzte Sili¬ kon hydrophil zu machen. Nachteilig an den diese Fluortenside 5 enthaltenden Zusammensetzungen ist jedoch, daß die Fluortenside das Überlackieren des vernetzten Silikons verhindern oder zu¬ mindest erheblich erschweren.In addition, US Pat. No. 4,657,959 describes compositions of different wettable silicone prepolymers based on siloxanes which contain ethoxylated, nonionic surfactants or fluorosurfactants. These surfactants serve to make the silicone crosslinked later hydrophilic. A disadvantage of the compositions containing these fluorosurfactants 5 is, however, that the fluorosurfactants prevent or at least considerably complicate the overpainting of the crosslinked silicone.

Aufgabe der Erfindung ist es, die genannten Nachteile zu ver- 10 meiden und Zusammensetzungen auf Basis silanmodifizierter Prä¬ polymere zur Verfügung zu stellen, die zu einem vernetzten Poly¬ mer führen, dessen Oberflächenklebrigkeit erheblich vermindert ist, daß aber trotzdem mit wäßrigen Dispersionen gut überlak- kierbar ist. 15The object of the invention is to avoid the disadvantages mentioned and to provide compositions based on silane-modified prepolymers which lead to a crosslinked polymer, the surface tack of which is considerably reduced, but which is nevertheless overlaid with aqueous dispersions - can be. 15

Ferner liegt der Erfindung die Aufgabe zugrunde, die Verminde¬ rung der Oberflächenklebrigkeit bei Erhaltung der guten Über- lackierbarkeit durch ein einfach handhabbares und kommerziell erhältliches Additiv zu ermöglichen. 20The invention is also based on the object of making it possible to reduce the surface tack while maintaining good paintability by means of an easy-to-handle and commercially available additive. 20th

Das Problem wird erfindungsgemäß durch Zusammensetzungen gelöst, die verzweigte oder unverzweigte, an den Kettenenden silanmodi¬ fizierte Präpolymere und Fluortenside enthalten.According to the invention, the problem is solved by compositions which contain branched or unbranched prepolymers and fluorosurfactants which are silane-modified at the chain ends.

25 Als silanmodifizierte Präpolymere können beispielsweise die in der US-PS 3 971 751 beschriebenen, unverzweigten Präpolymere mit der nachstehend aufgeführten allgemeinen Formel:25 For example, the unbranched prepolymers described in US Pat. No. 3,971,751 with the general formula listed below can be used as silane-modified prepolymers:

(R' )3_aRaSi-(CH2)3-O-(CH2-CH-0)n-(CH2)3)-SiRa(R' )3.a 30 I(R ') 3 _ a R a Si- (CH 2 ) 3 -O- (CH 2 -CH-0) n - (CH 2 ) 3 ) -SiR a (R') 3 . a 30 I

CH3 CH 3

verwendet werden, worin R und R' Alkyl-, Alkoxy-, Aminoxy-, Säureamid- oder Ketoximatogruppen sind, n eine Zahl von 1 bis 35 500, insbesondere von 100 bis 300 ist und a eine Zahl von 0 bis 2 ist, wobei mindestens eine hydrolisierbare Gruppe direkt an das Si-Atom gebunden ist. Bevorzugt ist, daß R eine verzweigte oder unverzweigte C-C10- Alkylgruppe, besonders bevorzugt eine Cx-Cs-Alkylgruppe und insbesondere eine Methylgruppe ist und R' eine Alkoxygruppe, eine Ketoximatogruppe, eine Aminoxygruppe, besonders bevorzugt eine Alkoxygruppe mit der Struktur OR" ist, wobei R" eine C!-C10- Alkylgruppe, besonders bevorzugt eine Ci-Cs-Alkylgruppe und insbesondere eine Methylgruppe ist.are used, wherein R and R 'are alkyl, alkoxy, aminoxy, acid amide or ketoximato groups, n is a number from 1 to 35,500, in particular from 100 to 300 and a is a number from 0 to 2, where at least a hydrolyzable group is bonded directly to the Si atom. It is preferred that R is a branched or unbranched CC 10 alkyl group, particularly preferably a Cx-Cs-alkyl group and in particular a methyl group and R 'is an alkoxy group, a ketoximato group, an aminoxy group, particularly preferably an alkoxy group with the structure OR ", where R "is a C ! -C 10 - alkyl group, particularly preferably a Ci-Cs alkyl group and in particular a methyl group.

Erfindungsgemäß werden als Additive gegenüber dem silanmodifi- zierten Präpolymeren inerte, feste oder flüssige, gesättigte Fluorverbindungen verwendet, die auch als Fluortenside bekannt sind. Vorzugsweise werden aliphatische Fluortenside eingesetzt. In ihrem chemischen Aufbau entsprechen sie fluorierten Alkyl(poly)alkoxylaten, fluoriertenAlkyl(poly)sulfonamiden oder Mischungen davon. Verbindungen dieser Art werden z.B. unter den Bezeichnungen Fluorad® bzw. Dynamar® von der Firma 3M vertrieben. Gegebenenfalls können diese Fluortenside mit weiteren Fluorver¬ bindungen gemischt werden. Die erfindungsgemäßen Zusammensetzun¬ gen enthalten 0,01 bis 10 Gew.%, insbesondere 0,05 bis 5 Gew.% Fluorverbindungen, bezogen auf das Gewicht der Zusammensetzun¬ gen.According to the invention, inert, solid or liquid, saturated fluorine compounds, which are also known as fluorosurfactants, are used as additives with respect to the silane-modified prepolymer. Aliphatic fluorosurfactants are preferably used. In their chemical structure they correspond to fluorinated alkyl (poly) alkoxylates, fluorinated alkyl (poly) sulfonamides or mixtures thereof. Compounds of this type are sold under the names Fluorad ® or Dynamar ® by 3M for example. If appropriate, these fluorosurfactants can be mixed with further fluorine compounds. The compositions according to the invention contain 0.01 to 10% by weight, in particular 0.05 to 5% by weight, of fluorine compounds, based on the weight of the compositions.

Die erfindungsgemäßen Zusammensetzungen können eine oder mehrere unverzweigte oder verzweigte silanmodifizierte Präpolymerkom- ponenten und ferner gegebenenfalls andere Polymere oder Präpoly¬ mere enthalten. Außerdem können weitere Additive wie Weichma¬ cher, Füllstoffe, Silane, Antioxidantien, Farbstoffe oder Kata¬ lysatoren in den Zusammensetzungen enthalten sein.The compositions according to the invention can contain one or more unbranched or branched silane-modified prepolymer components and further optionally other polymers or prepolymers. In addition, other additives such as plasticizers, fillers, silanes, antioxidants, dyes or catalysts can be present in the compositions.

Die erfindungsgemäßen Zusammensetzungen werden durch Vermischen der Präpolymeren mit den Fluorverbindungen und gegebenenfalls unter Zusatz weiterer, oben angegebener Additive hergestellt. Vorzugsweise erfolgt der Zusatz der Fluorverbindungen bereits am Anfang der Mischungsherstellung. Sollten feste Fluorverbindungen eingesetzt werden, ist es gegebenenfalls zweckmäßig, diese in einem Weichmacher oder einem Lösungsmittel vorzulösen bzw. anzu- pasten, um eine schnelle und homogene Verteilung im Präpolymer zu gewährleisten.The compositions according to the invention are prepared by mixing the prepolymers with the fluorine compounds and, if appropriate, with the addition of further additives specified above. The fluorine compounds are preferably added at the beginning of the preparation of the mixture. If solid fluorine compounds are used, it may be advisable to pre-dissolve them in a plasticizer or a solvent. paste to ensure a quick and homogeneous distribution in the prepolymer.

Obwohl durch Zugabe von Fluortensiden im allgemeinen, so z.B. auch bei Silikon-Dichtmassen, eine Uberlackierung mit wäßrigen Dispersionen erschwert oder ganz unmöglich gemacht wird, beein¬ trächtigen die Fluorverbindungen in den erfindungsgemäßen Zu¬ sammensetzungen die Überlackierbarkeit nicht. Durch das Fehlen von Siloxanoligomeren sind die erfindungsgemäßen Dichtmassen auch absolut "verfärbungsfrei" .Although by adding fluorosurfactants in general, e.g. Even in the case of silicone sealing compounds, overpainting with aqueous dispersions is made difficult or completely impossible, the fluorine compounds in the compositions according to the invention do not impair the ability to be painted over. Due to the lack of siloxane oligomers, the sealing compounds according to the invention are also absolutely "free from discoloration".

In der Tabelle sind zur näheren Erläuterung der Erfindung drei typische Rezepturen aufgeführt. Rezeptur A ist ein Vergleichs¬ beispiel, das kein Fluortensid enthält. Rezeptur C enthält im Unterschied zu Rezeptur B neben 30 % des silanmodifizierten Prä¬ polymeren auch 5 % Polyvinylchlorid. Die Angaben sind jeweils in Gew.%.In the table, three typical formulations are listed for a more detailed explanation of the invention. Recipe A is a comparative example that contains no fluorosurfactant. In contrast to formulation B, formulation C contains, in addition to 30% of the silane-modified prepolymer, 5% of polyvinyl chloride. The figures are in% by weight.

Tabelle 1Table 1

Figure imgf000007_0001
Figure imgf000007_0001

*Bis[3-(methyldimethoxysilyl)propyl]polyoxypropylen* Bis [3- (methyldimethoxysilyl) propyl] polyoxypropylene

**Paste aus 50 Teilen Dioctylphthalat und 50 Teilen Fluortensid. Nach der Mischungsherstellung wurden die Zusammensetzungen A, B und C auf Glas- bzw. Polyethylenplatten oder lackierte Hölzer aufgetragen, um Haftung, Shore-A-Härte, Durchhärtegeschwindig- keit und Oberflächenklebrigkeit zu prüfen. Die Ergebnisse sind in Tabelle 2 zusammengefaßt.** Paste of 50 parts dioctyl phthalate and 50 parts fluorosurfactant. After the mixture had been produced, compositions A, B and C were applied to glass or polyethylene plates or lacquered wood in order to test adhesion, Shore A hardness, through-hardening speed and surface tack. The results are summarized in Table 2.

Tabelle 2Table 2

BB

+ + + + 27 26+ + + + 27 26

3 33 3

+ ++ +

0,39 abesL0.39 abesL

Figure imgf000008_0001
Figure imgf000008_0001

Die Oberflächenklebrigkeit wird bestimmt, indem eine Stahlkugel mit einem Durchmesser von 3 mm auf das Ende eines ca. 2 mm star- ken Feldes der ausvulkanisierten Zusammensetzung gelegt wird, das auf einer beweglichen Platte (L = 40 cm) befestigt ist. An der Seite, an der sich die Kugel befindet, wird die Platte lang¬ sam hochgehoben. Es wird die Höhe H bestimmt, bei der die Kugel die entstandene schiefe Ebene hinabzurollen beginnt. Je kleb- riger die Oberfläche der zu testenden Zusammensetzung ist, desto höher muß das Ende der Platte gehoben werden, bevor die Kugel in Bewegung gerät. Die Kugel wird daher um so eher ins Rollen gera¬ ten, je weniger Tack die ausvulkanisierte Zusammensetzung auf¬ weist, d.h. desto niedriger sind die erhaltenen Werte für H. Aus Tabelle 2 erkennt man, daß durch den Zusatz des erfindungsgemä¬ ßen Fluortensids eine deutliche Reduzierung der Öberflächenkleb- rigkeit erzielt werden kann. Der Rollbeginn von ca. 5 cm liegt hierbei in der Größenordnung, wie er auch mit neutralvernetzen¬ den Silikonen erreicht wird.The surface stickiness is determined by placing a steel ball with a diameter of 3 mm on the end of an approximately 2 mm thick field of the vulcanized composition, which is attached to a movable plate (L = 40 cm). On the side on which the ball is located, the plate is slowly lifted up. The height H at which the ball begins to roll down the resulting inclined plane is determined. The more sticky the surface of the composition to be tested, the higher the end of the plate has to be lifted before the ball starts to move. The ball will therefore start rolling the sooner the less tack the vulcanized composition has, ie the lower the values obtained for H. From Table 2 it can be seen that the addition of the fluorosurfactant according to the invention results in a clear reduction Reduction of surface adhesive can be achieved. The start of rolling of about 5 cm is of the order of magnitude that is also achieved with neutral cross-linking silicones.

Die erfindungsgemäßen Fluortenside können selbstverständlich neben ihrem Einsatz in Einkomponenten-Systemen, wie in den Bei¬ spielen A bis C gezeigt ist, auch in Mehr-, vorzugsweise in Zweikomponenten-Systemen verwendeten werden. Unter letzteren versteht man Systeme, bei denen die Härtung nicht durch eindif- fundierende Luftfeuchtigkeit sondern durch Vermischen von zwei oder mehr Komponenten bewerkstelligt wird. In addition to their use in one-component systems, as shown in Examples A to C, the fluorosurfactants according to the invention can of course also be used in multi-component, preferably in two-component systems. The latter is understood to mean systems in which the hardening is accomplished not by diffusing air humidity but by mixing two or more components.

Claims

Patentansprüche Claims 1. Zusammensetzungen dadurch gekennzelchnel:, daß sie verzweigte oder unverzweigte, an den Kettenenden silanmodifizierte1. Compositions characterized in that they branched or unbranched, silane-modified at the chain ends Präpolymere und Fluortenside enthalten.Contain prepolymers and fluorosurfactants. 2. Zusammensetzungen nach Anspruch 1, dadurch gekennzeichnet, daß die silanmodifizierten Präpolymere die allgemeine For- mel:2. Compositions according to claim 1, characterized in that the silane-modified prepolymers have the general formula: (R')3_aRaSi-(CH2)3-0-(CH2-CH-0)n-(CH2)3)-SiRa(R')3.a (R ') 3 _ a R a Si- (CH 2 ) 3 -0- (CH 2 -CH-0) n - (CH 2 ) 3 ) -SiR a (R') 3 . a II. CH3 CH 3 besitzen, worin R und R' Alkyl-, Alkoxy-, Aminoxy-, Säure- amid- oder Ketoximatogruppen sind, n eine Zahl von 1 bis 500 und a eine Zahl von 0 bis 2 ist.have where R and R 'are alkyl, alkoxy, aminoxy, acid amide or ketoximate groups, n is a number from 1 to 500 and a is a number from 0 to 2. 3. Zusammensetzungen nach Anspruch 1 oder 2, dadurch gekenn¬ zeichnet, daß n eine Zahl von 100 bis 300 ist.3. Compositions according to claim 1 or 2, characterized gekenn¬ characterized in that n is a number from 100 to 300. 4. Zusammensetzungen nach einem der Ansprüche 1 bis 3, dadurch gekennzeichnet, daß die Fluortenside aliphatische Fluorten- side sind.4. Compositions according to one of claims 1 to 3, characterized in that the fluorosurfactants are aliphatic fluoride side. 5. Zusammensetzungen nach einem der Ansprüche 1 bis 4, dadurch gekennzeichnet, daß die Fluortenside fluorierte Alkyl(po- ly)alkoxylate, fluorierte Alkyl(poly)sulfonamide oder Mi- schungen davon sind und gegebenenfalls mit weiteren Fluor¬ verbindungen vermischt sind.5. Compositions according to one of claims 1 to 4, characterized in that the fluorosurfactants are fluorinated alkyl (poly) alkoxylates, fluorinated alkyl (poly) sulfonamides or mixtures thereof and are optionally mixed with further fluorine compounds. 6. Zusammensetzungen nach einem der Ansprüche 1 bis 5, dadurch gekennzeichnet, daß sie Fluorverbindungen in einer Menge von 0,01 bis 10 Gew.% enthalten. 6. Compositions according to one of claims 1 to 5, characterized in that they contain fluorine compounds in an amount of 0.01 to 10 wt.%. 7. Zusammensetzungen nach einem der Ansprüche 1 bis 6, dadurch gekennzeichnet, daß sie Fluorverbindungen in einer Menge von 0,05 bis 5 Gew.% enthalten.7. Compositions according to one of claims 1 to 6, characterized in that they contain fluorine compounds in an amount of 0.05 to 5 wt.%. 8. Zusammensetzungen nach einem der Ansprüche 1 bis 7, dadurch gekennzeichnet, daß sie eine oder mehrere silanmodifizierte Präpolymerkomponenten und gegebenenfalls andere Polymere oder Präpolymere enthalten.8. Compositions according to one of claims 1 to 7, characterized in that they contain one or more silane-modified prepolymer components and optionally other polymers or prepolymers. 9. Zusammensetzungen nach einem der Ansprüche 1 bis 8, dadurch gekennzeichnet, daß sie weitere Additive wie Weichmacher, Füllstoffe, Silane, Antioxidantien, Farbstoffe oder Kataly¬ satoren enthalten.9. Compositions according to one of claims 1 to 8, characterized in that they contain further additives such as plasticizers, fillers, silanes, antioxidants, dyes or catalysts. 10. Verfahren zur Herstellung einer Zusammensetzung gemäß einem der Ansprüche 1 bis 9, dadurch gekennzeichnet, daß die Flu¬ ortenside und die Präpolymeren einfach vermischt werden.10. A method for producing a composition according to any one of claims 1 to 9, characterized in that the fluorosurfactants and the prepolymers are simply mixed. 11. Verfahren nach Anspruch 10, dadurch gekennzeichnet, daß die Fluortenside gleich am Anfang des Vermischens zugesetzt werden und gegebenfalls vorher in einem Weichmacher oder einem Lösungsmittel angeteigt oder gelöst werden.11. The method according to claim 10, characterized in that the fluorosurfactants are added right at the beginning of the mixing and, if necessary, pasted or dissolved beforehand in a plasticizer or a solvent. 12. Verwendung der Zusammensetzungen gemäß einem der Ansprüche 1 bis 9 als Kleb- und/oder Dichtstoff.12. Use of the compositions according to one of claims 1 to 9 as an adhesive and / or sealant. 13. Verwendung von Fluortensiden in Zusammensetzungen auf Basis silanmodifizierter Präpolymere zur Verringerung der Ober¬ flächenklebrigkeit bei gleichzeitigem Erhalt der guten Über- lackierbarkeit mit wässrigen Dispersionsfärben. 13. Use of fluorosurfactants in compositions based on silane-modified prepolymers to reduce the surface stickiness while at the same time maintaining good paintability with aqueous dispersion colors.
PCT/EP1992/001194 1991-06-13 1992-05-31 Sealants and adhesives based on silane-modified prepolymers Ceased WO1992022609A1 (en)

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