Patent GB-956363-A (GB)
Title: The use of organic-silicon compounds in resin-filler compositions
IPC: C03C25/40
Filed: 1960-07-11
Abstract: Composite articles are prepared by curing a mixture of a thermosetting resin, an inorganic oxygen-containing filler material and an amino-alkyl-silicon compound containing the group: <FORM:0956363/C3/1> where R is a divalent saturated hydrocarbon group containing up to 10 carbon atoms, A is hydrogen, alkyl or aryl, and a is at least 3, the non-primary nitrogen atom being separated from the silicon by at least 3 carbon atoms, and at least one free valency of the silicon being connected to an alkoxy group or to a silicon atom through an oxygen atom.  The organoisilicon compound may first be mixed with either of the other two ingredients before adding the third, and such combinations are claimed.  The silicon compounds may be either silanes or polysiloxanes. In the silanes, the remaining groups attached to silicon are specifically R1y(OR11)3-y, where y is 0, 1 or 2, R1 is alkyl or aryl and R11 is alkyl.  The polysiloxanes have the formula: <FORM:0956363/C3/2> or may be copolymers including conventional units.  The organosilicon compounds are described in Specification 882,051. The thermosetting resin is preferably an aldehyde condensation resin, an epoxy resin or a polyurethane. Aldehyde condensates include phenol-, cresol-, urea- and mealmine-aldehyde resins. The epoxy resins include diglycidyl ethers of polyhydric phenols and blends thereof with polyphenols. The inorganic filler material may be fibres, mats, rovings and particulate materials made from oxides, silicates, aluminates and carbonates, e.g., glass, asbestos, mica, quartz, calcium carbonate, iron oxide, kieselguhr and diatomaceous earth. For treating such a filler, the silicon compound is dissolved in a solvent which may be water and/or an alcohol or ether alcohol, or an aromatic hydrocarbon. Such solutions may also be used for mixing with the thermosetting resin. Preferably, a small amount of an organic acid, e.g. acetic, is added to the solutions. The invention is illustrated only with glass cloth for making laminates (see Division B5). The specific silicon compounds are N-gamma-aminopropyl-delta-aminobutyl-triethoxy silane, N-beta-aminoethyl-gamma - aminoisobutyl - methyldiethoxy silane, N - beta - aminoethyl - gamma - aminopropyltriethoxy silane and a copolymer of N-beta-aminoethyl - gamma - aminoisobutylmethyl siloxane and dimethyl siloxane.  The aminoalkyl-substituted aminoalkyl silicon compounds may be prepared by reacting aliphatic diamines with a chloroalkyl alkoxy silane or chloroalkyl polysiloxane or by hydrogenating cyanoalkyl-amino-alkyl silicon compounds.ALSO:An inorganic oxygen-containing filler material, which may be in the form of fibres, mats, cloth, rovings and particulate or pulverulent material, is coated with an organosilicon compound containing the group <FORM:0956363/B1-B2/1> where R is a divalent saturated hydrocarbon group containing up to 10 carbon atoms, A is hydrogen, alkyl or aryl, and a is at least 3, the non-primary nitrogen atom being separated from the silicon by at least 3 carbon atoms, and at least one free valency of the silicon being connected to an alkoxy group or to a silicon atom through an oxygen atom; these compounds may be silanes or polysiloxanes.  Subsequently a thermosetting resin such as a phenol-aldehyde or amine-aldehyde resin or an epoxy or urethane resin is applied and the composite bodies are cured.  The preferred filler material is glass cloth from which laminates are prepared.  Other fillers specified are oxides, silicates, aluminates and carbonates, e.g. other forms of glass, asbestos, mica, quartz, calcium carbonate, iron oxide, kieselguhr and diatomaceous earths. The coating is preferably effected in a solution of organosilicon compound to which a small amount of an organic acid, e.g. acetic acid, has been added.  The specific organo-silicon compounds are typified by N-gamma-aminopropyl-delta-aminobutyl-triethoxy silane and a copolymer of N-beta-aminoethyl-gamma-aminoisobutylmethylsiloxane and dimethylsiloxane.  Alternatively a mixture of the siloxane and the other resin may be applied.  Specification 882,051 is referred to.ALSO:Fibrous inorganic oxygen-containing filler materials, e.g glass and asbestos, are coated with a silane or polysiloxane containing the group <FORM:0956363/D1-D2/1> where R is a divalent saturated hydrocarbon group containing up to 10 carbon atoms, A is hydrogen, alkyl or aryl, and a is at least 3, the non-primary nitrogen atom being separated from the silicon by at least 3 carbon atoms; in the silanes, at least one free valency of the silicon is connected to an alkoxy group. Subsequently, or simultaneously, a thermosetting resin is applied and the composite bodies are curved. The coating is preferably effected in a solution of the organosilicon compound to which a small amount of an organic acid, e.g. acetic, has been added.  The specific organosilicon compounds are typified by N-gamma-aminopropyl-delta-aminobutyl-triethoxy silane and a copolymer of N-beta-aminoethyl-gamma-aminoisobutyl methyl siloxane. Specification 882,051 is referred to.