Abstract: The properties of polyphenylene ether-polyamide mixtures can be improved by the addition of polysiloxane compounds.

Abstract: The invention describes a process for the production of a composite article of at least two component pieces, firmly bonded to one another, of a vulcanized rubber compound on the one hand and a polyamide composition on the other hand, the vulcanized rubber compound being prepared under customary vulcanization conditions in contact with the polyamide composition by vulcanization of a rubber compound which comprises the following components:I. 100 parts by weight of a rubber,II. 0 to 300 parts by weight of fillers,III. 0 to 150 parts by weight of plasticizer,IV. 1 to 10 parts by weight of peroxide vulcanization agent,V. 0 to 4 parts by weight of vulcanization activators andVI. 1 to 10 parts by weight of a silane containing double bonds.

Abstract: The capping of anionic polymers to make functionalized polymers is improved by using alkoxy silyl compounds having protected functional groups, such as acetal groups, as the capping agent. The protected functional groups are stable under a variety of conditions and then readily convert to more reactive terminal functional groups useful for making adhesives, sealants and coatings.

Abstract: Fluoroinfused composites exhibiting low surface energy and low kinetic coefficent of energy are prepared via contact of a swellable polymeric material with a solution comprising a swelling solvent, an organofluorosilane and a gelling agent.

Abstract: Crosslinkable and crosslinked compositions comprising silicon compounds, unsaturated elastomeric polymers and polyenes. Along with, or instead of these polyenes and silicon compounds, crosslinkable prepolymers prepared from such polyenes and silicon compounds may be included. Crosslinking, of the crosslinkable compositions, may be accomplished by hydrozilation, in the presence of hydrosylation catalysts.

Abstract: A method for producing asymmetric radial polymers which comprises anionically polymerizing an anionically polymerizable monomer to form a first set of living polymer arms, coupling the first set of living polymer arms with a silicon-based coupling agent, substantially completing the coupling reaction, anionically polymerizing, in the presence of the coupled first set of polymer arms, a different anionically polymerizable monomer(s) to form a second set of living polymer arms, and adding a coupling activator and coupling the second set of living polymer arms to the coupled first set of polymer arms to form the asymmetric radial polymer.

Abstract: The present invention is a bituminous roofing composition which is especially useful to coat and/or saturate a roll roofing membrane. The composition comprises from 2 to 10 percent by weight, based on block copolymer plus bitumen, of a block copolymer of a vinyl aromatic hydrocarbon and a conjugated diene, from 25 to 300 parts by weight per hundred parts of said block copolymer of an endblock compatible resin which has a softening point above 100.degree. C., and the balance being a bituminous material. Preferably, the solubility parameter of the endblock resin is within 0.3 [cal/cm.sup.3 ].sup.1/2 of that of the vinyl aromatic hydrocarbon portion of the block copolymer.

Abstract: A process is disclosed for producing six-armed and eight-armed asymmetric radial block copolymers. The process comprises anionically polymerizing a diene and/or a vinyl aromatic hydrocarbon to create living polydiene and/or vinyl aromatic hydrocarbon arms, sequentially anionically polymerizing a vinyl aromatic hydrocarbon and a diene to create living block copolymer arms and coupling the two sets of arms together in one step with a coupling agent that will couple six or eight arms, wherein the molar ratio of the vinyl aromatic hydrocarbon-diene arms to the polydiene arms is sufficient to produce a statistical blend with less than 5 weight percent homopolydiene.

Abstract: Polyolefin molding composition of high rigidity and hardnessA polyolefin molding composition essentially comprisinga) a polyolefin wax andb) a high-molecular-weight polyolefin or, instead of b),c) a high-molecular-weight olefin copolymer has high rigidity and hardness.In order to increase the impact strength, this molding composition may additionally be admixed with a rubber having a glass transition temperature of below -20.degree. C.

Abstract: A curable composition which comprises (C) a non-polymeric organic curing agent having at least two hydrosilyl groups in a molecule, (D) an organic polymer having at least one alkenyl group in a molecule, and (E) a hydrosilylation catalyst has rapid curability and good depth curability, and gives a homogeneous cured material having good mechanical properties.

Abstract: Fluid gasket composition with fine rubber particles has sufficient elasticity. The particle size of the rubber particles contained in the fluid gasket composition is desired to be 0.1 to 3.0 mm. The fluid gasket composition applied to a joint portion between mechanical parts or the like exhibits an effect of sealing and absorbing vibrations, dislocation and mechanical movements taking place in the mechanical parts.

Abstract: An adhesive silicone rubber composition of addition reaction curing type comprising (a) an organopolysiloxane containing an alkenyl group; (b) an organohydrogenpolysiloxane having at least one hydrogen atom directly attached to a silicon atom in a molecule; (c) an addition reaction catalyst; and (d) an adhesive agent selected from compounds of the following formulae (I), (II) and (III):A-(D-B).sub.x -D-A (I)C-(B-D).sub.

Abstract: A composition useful in the fabrication of extruded articles contains a thermoplastic resin such as polyethylene and from 100-3,000 parts per million of a lubricant which is (i) an organosilicon resinous copolymer having a number average molecular weight of between 1,200-10,000 and R.sub.3 SiO.sub.1/2, R.sub.2 SiO.sub.2/2, RSiO.sub.3/2 and SiO.sub.4/2 units, wherein R is a C.sub.1 -C.sub.6 alkyl, aryl, alkenyl and/or trifluoropropyl radical(s); or (ii) the organosilicon resinous copolymer and a siloxane polymer R.sub.3 SiO(R.sub.2 SiO).sub.n SiR.sub.3 wherein R is as defined heretofore and n is 1-100,000; or (iii) the organosilicon resinous copolymer and an absorbing filler such as silica; or (iv) the organosilicon resinous copolymer, the siloxane polymer and an absorbing filler.

Abstract: A free-flowing silicone polymer powder, having an average particle size of 1 to 1000 microns and prepared by mixing a polydiorganosiloxane with a silica filler, is uniformly dispersed in an organic resin using conventional equipment, such as a single screw or, preferably, a twin screw extruder. When employed at a concentration of about 0.5 to 25 parts by weight of powder per 100 parts by weight of resin, a significant improvement in the burn character of the modified resin is obtained such that the rate of heat release, generation of smoke and evolution of toxic carbon monoxide gas is significantly reduced relative to the unmodified resin.

Abstract: Polymer particles including polysiloxane is disclosed. The polymer particles are prepared by condensing at least one organosilane or organosiloxane compound in the presence of organic polymer particles which are prepared from specific monomers and dispersed in an aqueous medium. The polymer particles possess excellent water resistance, weatherability, water repellency, adhesion, and flexing resistance, and thus are useful as water paints, coating agents, carpet packing material, floor polishing agents, cementing medium, and the like.

Abstract: A release agent comprising a resin containing siloxane segments is described. The resin has been modified with a silane coupling agent containing at least one free isocyanate group and contains one or more hydrolyzable silyl groups in side chains of its molecule.

Abstract: A curable composition comprising(A) a vinyl resin having at least one hydrolyzable silyl group in one molecule wherein the main chain substantially consists of a vinyl polymer and having no segment of a resin which has polymerizable double bonds at both ends of the main chain and a glass transition temperature of not more than 0.degree. C.;(B) a modified resin having at least one hydrolyzable silyl group in one molecule which is obtained by polymerizing(a) a resin having polymerizable double bonds at both ends of the main chain and a glass transition temperature of not more than O.degree. C.,(b) a hydrolyzable silyl group-containing vinyl monomer, and(c) a vinyl monomer having no hydrolyzable silyl group; and(C) a curing catalyst. The composition of the present invention enables to prepare a top coating having the excellent physical property balance between hardness and impact resistance or that between elongation and stain resistance.

Abstract: Fully alkoxysilane-functionalized aliphatic polyamine compounds (e.g., fully functionalized dialkylenetriamine compounds) can be formed by reacting a dialkylenetriamine (e.g., diethylenetriamine) with a compound comprising an amine-reactive group and an alkoxysilane group (e.g., an isocyanatoalkylalkoxysilane). These functionalized compounds find utility as the predominant component in forming organic/inorganic hybrid materials via sol-gel processing.

Abstract: A method for preparing asymmetric radial polymers wherein the different polymeric arms are contacted sequentially with a coupling agent. The method narrows the relative arm distribution of the several asymmetric radial polymers produced and significantly increases the amount of total product having the desired ratio of polymeric arms. Any coupling agent known in the prior art to be useful in the production of asymmetric radial polymers may be used in the method of this invention but coupling agents having from three to about twelve functional groups are most effective.

Abstract: The present invention utilizes a class of novel hydrosilation catalysts that are inhibited in the absence of molecular oxygen to prepare storage stable, one part curable compositions containing (1) compounds with alkenyl radicals and (2) compounds with silicon-bonded hydrogen atoms. The compositions are stable until exposed to molecular oxygen, at which time they cure in the same manner as conventional compositions containing these ingredients.

Abstract: A process for making a fluorinated copolymer is disclosed. The process comprises polymerizing a monomer to form a polymer and then terminating the polymerization by adding a perfluorinated alkyl chlorosilane to the polymer. The perfluorinated alkyl chlorosilane reacts with the polymer to form a copolymer having a fluorinated terminal portion thereon.

Abstract: There are disclosed novel, solid, elastomeric block copolymers with improved resistance to cold flow wherein either 1) the terminal blocks are polymers of at least one conjugated diene I, e.g., isoprene, which contains at least five carbon atoms with at least one of each pair of double-bonded carbon atoms in the polymerized diene I units being additionally single-bonded to two carbon atoms, at least one middle or interior block is a polymer of butadiene, and at least one middle or interior block is a polymer of at least one aryl-substituted olefin, e.g., styrene; or 2) the terminal blocks are random copolymers of at least one diene I as previously defined and butadiene, and at least one middle or interior block is a polymer of at least one aryl-substituted olefin.

Abstract: A novel method is proposed for the effective utilization of scraps of cured silicone rubbers, of which no method of disposal is known heretofore other than discarding as a waste material. Namely, scraps of cured silicone rubbers can be compounded in a considerably large amount with a vulcanizable composition based on an organic rubbery elastomer such as fluorocarbon rubbers, e.g., binary copolymers of hexafluoropropylene and vinylidene fluoride, and dispersed therein in such fineness that particles of the cured silicone rubber can no longer be recognized by the naked eyes only when the organic rubbery elastomer composition has a specific Mooney viscosity (ML.sub.1+4 100.degree. C.) of at least 70 to give a uniform curable rubber composition capable of being cured into vulcanized rubber articles having various properties as good as or comparable with those of the vulcanized rubber articles from the same organic rubbery elastomer without admixture of cured silicone rubber scraps.

Abstract: Polymeric stabilizers with a polysiloxanic structure contain sterically hindered phenol groups and reactive groups capable of binding themselves to the polymeric structure to be stabilized. These polymeric stabilizers are particularly suitable for applications which require the non-extractability of additives due to solvents, fats or soaps.

Abstract: The present invention provides a copolymer comprising polybutadiene and other olefinic saturated or unsaturated thermoplastics. The mixing ratio between the polybutadiene and the thermoplastics is 30:70 to 95:5 weight percent. Surface improving additives, such as polysiloxane, may be added in quantities from 0.5 to 6 weight percent. The copolymer may be used to produce medical and food compatible semi-finished or finished products.

Abstract: A substrate is provided with a release surface by application of an emulsion of a vinyl-addition silicone system and catalyst therefor and a particulate component, preferably a resin. The vinyl addition silicone system is cured upon application of heat and removal of water.

Abstract: A method for preparing tapered block copolymers in a polymerization process by charging an initiator and monomers sequentially with one or more charges of first one of the monomers, then with a mixture of the two monomers, and then with one or more charges of the second monomer alternating with one or more charges of the first monomer with subsequent coupling to produce a polymodal tapered block copolymer. Suitable monomers include conjugated dienes and monovinylaromatic compounds. The copolymers are suitable for use in injection and blow molding equipment; the copolymers are particularly useful for shrink films, containers, tubes, fibers and other packaging applications.

Abstract: A series of new high abrasion resistance coating materials have been prepared utilizing organic/inorganic hybrid materials formed by cohydrolyzing a metal alkoxide sol (e.g. silicon, aluminum, titanium, or zirconium metal alkoxide sol) with one or more bis(trialkoxysilane-containing) organic components or related functionalized species. These hybrid materials show optical clarity and improve the abrasion resistance of polymer substrates when applied as coatings and cured on such substrates.

Abstract: A hydrogenated diene block copolymer having a polystyrene-reduced number-average molecular weight of 50,000-600,000 which is a hydrogenation product of an (A)-(B) block copolymer in which (A) means an alkenyl aromatic compound polymer block and (B) means a conjugated diene homopolymer block wherein the vinyl content of the conjugated diene portion is more than 60%, or an alkenyl aromatic compound-conjugated diene random copolymer block wherein the vinyl content of the conjugated diene portion is 15% or more, an (A)-(B)-(C) block copolymer in which (A) and (B) are as defined above and (C) means an alkenyl aromatic compound-conjugated diene copolymer tapered block wherein the proportion of the alkenyl aromatic compound increases gradually, or an (A)-(B)-(A) block copolymer in which (A) and (B) are as defined above and in which hydrogenation product at least 80% of the double bonds of the conjugated diene portion is saturated by the hydrogenation.

Abstract: A method for producing, in the presence of both monomers, a block copolymer of a polymer block of a vinyl aromatic hydrocarbon (and/or a conjugated diene) and a block of polydimethysiloxane which comprises adding a vinyl aromatic hydrocarbon, an organo alkali metal promoter, hexamethylcyclotrisiloxane and a polar promoter to a solvent (or to the styrene if no solvent is to be used) at a temperature of 0.degree. to 60.degree. C., allowing the polymerization of the vinyl aromatic hydrocarbon to proceed until the color of the vinyl aromatic hydrocarbon - Li.sup.+ species which is initially produced fades, then raising the temperature to 60.degree. to 120.degree. C. wherein the hexamethylcyclotrisiloxane polymerizes at the end of the polystyrene polymer blocks and then terminating the polymerization.

Abstract: The present invention is an improvement upon the process for making block copolymers of vinyl aromatic hydrocarbons and/or conjugated dienes, and polydimethylsiloxane by first anionically polymerizing the vinyl aromatic hydrocarbon to make a living polymer block and then adding hexamethylcyclotrisiloxane and a polar promoter to polymerize a polydimethylsiloxane block at the end of the living polymer block. The improvement comprises reacting the living polymer blocks with a crossover reagent to decrease the crossover time from the living polymer block polymerization to the polydimethylsiloxane polymerization.

Abstract: A star block copolymer comprised of vinyl aromatic hydrocarbon and/or conjugated diene polymer arms and polydimethylsiloxane arms radiating outwardly from a polyalkenyl aromatic coupling agent core is produced by first anionically polymerizing a vinyl aromatic hydrocarbon and/or a conjugated diene to produce living polymer arms, reacting the living polymer arms with a polyalkenyl aromatic coupling agent to couple the arms thereto, polymerizing this coupled product with hexa-methylcyclotrisiloxane in the presence of a polar promoter and then terminating the polymerization.

Abstract: A particulate polybutadiene crosslinked material is disclosed along with a process of making the same. The particulate material has a substantially spherical, uniformly shaped configuration and comprises at least part of its surface layer occupied by a reaction product of polybutadiene and a silicone compound.

Abstract: Coupling of block base copolymers terminated by a lithium atom of the typical formula S-B-Li, in which S is a monovinylaromatic hydrocarbon block and B is a conjugated diene block, by the use of at least one difunctional deactivating coupling agent and at least one polyfunctional deactivating coupling agent in a molar ratio such that the linear polymer obtained by coupling represents 65 to 95% by weight of the total polymer material obtained by coupling.

Abstract: Crosslinkable carbosilane polymer formulations are prepared from saturated or unsaturated carbosilane polymers containing reactive silicon hydride radicals in the polymer chain combined with polycyclic polyene crosslinkers having two or more double bonds that are reactive in the hydrosilation crosslinking reaction.

Abstract: The amount of solvent-extractable materials present in organosiloxane gels cured by a platinum-catalyzed hydrosilylation reaction can be reduced without sacrificing other desirable properties the gels when the curable composition used to prepare the gel comprise a first polydiorganosiloxane with vinyl or other ethylenically unsaturated hydrocarbon radicals only at the terminal positions, a second polydiorganosiloxane with silicon bonded hydrogen atoms only at the terminal positions and a crosslinking reactant containing at least three alkenyl radicals or silicon-bonded hydrogen atoms per molecule. The number of silicon-bonded hydrogen atoms or alkenyl radicals in excess of 2 per molecule of crosslinking reactant constitute from 10 to 30 percent of these reactive groups present in the curable composition.

Abstract: A moisture-crosslinkable primer which comprises a solution of a hydrogenated polybutadiene into which has been introduced a silyl group of the formula: ##STR1## wherein R is an alkyl group having 1 to 5 carbon atoms, R' is an alkoxy group having 1 to 5 carbon atoms or a halogen atom, and n is an integer of from 1 to 3, in an organic solvent, which has excellent heat-resistant adhesion and durable adhesion and is useful for adhering between polyolefinic substances or between polyolefinic substances and other organic substances.

Abstract: A polymeric ablative liner material based on carbon and silicone polymers and particulate fillers which is tailored to control the endothermic chemical reaction and thereby optimize the ablation process to provide maximum cooling and remaining char. The ablative liner material includes hydrocarbon polymers and has a molar ratio of carbon to silicon within the range of about 2 to 8. This composition optimizes the generation of gases for transpirational cooling, the cooling resulting from the endothermic chemical reaction, and the amount of stable char that remains after the ablation process is completed.

Abstract: A method for preparing asymmetric radial polymers wherein the different polymeric arms are contacted sequentially with a nonpolymerizable coupling agent. Contacting of the final step in the process, which frequently but not necessarily always will be the second step in the process, will be carried out in the presence of a polar compound suitable for increasing the amount of vinyl content in a conjugated diolefin polymer during polymerization thereof. The method used narrows the relative arm distribution of the several asymmetric radial polymers produced and significantly increases the amount of total product having the desired ratio of polymeric arms and accomplishes this objective in relatively short reaction time.

Abstract: The present invention relates to elastomeric copolymers and block copolymers, e.g., based upon styrene/isoprene, having a novel condensed phase structure wherein polymer branches occur along the polymer backbone, either at a predetermined location or at random locations. The polymers are made by a method which comprises the step of reacting, under polymerization conditions, hydrocarbyl lithium initiator, at least one anionically polymerizable compound, and an organometallic- substituted styrene condensing agent. The reactants may be added simultaneously to produce a copolymer with polymer branch segments randomly located along the polymer backbone or sequentially to produce a copolymer with branches located at the same predetermined location along the polymer backbone. The resultant polymers may be further reacted with a linking agent to form multi-arm copolymers.

Abstract: A modified organopolysiloxane comprising [R.sup.1.sub.2 SiO.sub.2/2 ] or [R.sup.1.sub.3 SiO.sub.1/2 ] units wherein R.sup.1 is a hydrogen atom or a monovalent hydrocarbon group having 1 to 12 carbon atoms, at least two R.sup.1 substituents per molecule being replaced by specific isocyanurate or cyanurate groups is a vulcanization activator for assisting in vulcanization of fluorocarbon rubber or fluorocarbon/silicon rubber compositions with peroxide vulcanizing agents. It is prepared by reacting triallyl isocyanurate, triallyl cyanurate or a derivative thereof with dimethylchlorosilane or methyldichlorosilane in the presence of a platinum catalyst to form a chlorosilane containing diallylisocyanurate or diallylcyanurate groups, followed by hydrolysis. An alternative process is by reacting triallyl isocyanurate, triallyl cyanurate or a derivative thereof with a siloxane in the presence of a platinum catalyst.

Abstract: A pressure-sensitive adhesive that can adhere aggressively to both polar and nonpolar substrates and has good internal strength at high temperatures is provided by heat or radiation curing a blend of an ethylenically-unsaturated .alpha.-olefin polymer, a crosslinker having at least 2 hydrosilyl groups, and a hydrosilation catalyst. A preferred hydrosilane crosslinker has the formula ##STR1## wherein R is an alkyl group having 1-6 carbon atoms, and n' is a number in the range of 2 to 35.

Abstract: A polylactone-modified organopolysiloxane compound, wherein a polylactone-containing group represented by the formula (I) is bound to a silicon atom located at at least either of the terminal positions and/or intermediate positions to impart excellent properties as a synthetic resin modifier (when Y in (I) is an acetyl group or a hydrogen atom) or as a film former (when Y in (I) is a hydrogen atom): ##STR1## wherein Z represents a trivalent hydrocarbon residue which may contain oxygen, sulfur or/and nitrogen atom(s); X represents a lactone group of the formula, ##STR2## (wherein R represents a hydrogen atom or an alkyl group containing from 1 to 12 carbon atoms; a represents an integer from 4 to 6), k and L each represents an integer of 1 or more; and Y represents a hydrogen atom or an acetyl group.

Abstract: This is an improvement in a process for the hydrogenation of conjugated diolefin polymers which comprises polymerizing or copolymerizing at least one conjugated diolefin with an organo alkali metal polymerization initiator in a suitable solvent thereby creating a living polymer, terminating the polymerization by the addition of hydrogen, thereby generating an alkali metal hydride, and effecting selective hydrogenation of the unsaturated double bonds in the conjugated diolefin units of the terminated polymer by contacting the polymer, in the absence of hydrocarbon lithium and alkoxy lithium compounds, with hydrogen in the presence of at least one bis(cyclopentadienyl)titanium compound. The improvement comprises treating the polymer, before hydrogenation, with a reagent to increase catalyst activity, the reagent being such that it will react with the alkali metal hydride present in the polymer.

Abstract: A silicone-based composite rubber composition having good processability on rolls which is obtained by compounding a rubber-forming polymer (A) comprising a polyorganosiloxane and an organic rubber, a silicon compound (B) having at least two hydrolyzable groups per molecule which are able to undergo hydrolysis and condensation reactions with silanols, and a heavy metal compound, amine, or quaternary ammonium salt (C) which catalyzes the hydrolysis and condensation reactions, and allowing the resulting formulation to undergo hydrolysis and condensation reactions while the formulation is kept being deformed by shearing; a crosslinkable, silicone-based composite rubber composition comprising the silicone-based composite rubber composition having blended therewith an organic rubber-crosslinking agent; and an oil seal and a rubber hose both obtained from the crosslinkable, silicone-based composite rubber composition.

Abstract: An oxygen-permeable transparent polymer composition for contact lenses of the rigid type comprises at least a first constituent having ethylene double bonds of the type which is polymerizable in a rigid matrix, and a second constituent formed by a silane monomer containing at least two silyl -SiH groups per molecule. The composition can include a third constituent of the polyorganosiloxysilane type.

Abstract: Rubber compositions are disclosed for integral attachment of polymeric and metallic materials. Improved bondability is attributed to the use of a selected base rubber blended with a selected class of inorganic or organic fillers, silane compounds and vulcanizing agents such that the finished composition is provided with a specified range of Mooney viscosities. Also disclosed is a method of hose-metal fitting connection by the application of the composition. Gas- and oil-impermeability characteristics are greatly enhanced.

Abstract: A surface-segregatable, melt-extrudable thermoplastic composition suitable for processing by melt extrusion to form a fiber or film having a differential, increasing concentration of an additive from the center of the fiber or film to the surface thereof, which differential, increasing concentration imparts to the surface of the fiber or film at least one desired characteristic which otherwise would not be present, which composition includes at least one thermoplastic polymer and at least one defined additive. During formation of the fiber or film, the additive rapidly segregates in a controllable manner toward the newly-formed surface of the fiber or film, thereby resulting in a controllable differential concentration of the polymeric material, which concentration increases with increasing distance from the center of the fiber or film to its surface. The weight ratio of the polymer to the additive is in the range of from about 1 to about 1,000.

Abstract: The present invention relates to elastomeric copolymers and block copolymers, e.g., based upon styrene/isoprene, having a novel condensed phase structure wherein polymer branches occur along the polymer backbone, either at a predetermined location or at random locations. The polymers are made by a method which comprises the step of reacting, under polymerization conditions, hydrocarbyl lithium initiator, at least one anionically polymerizable compound, and an organometallic-substituted styrene condensing agent. The reactants may be added simultaneously to produce a copolymer with polymer branch segments randomly located along the polymer backbone or sequentially to produce a copolymer with branches located at the same predetermined location along the polymer backbone. The resultant polymers may be further reacted with a linking agent to form multi-arm copolymers.

Abstract: A method for preparing asymmetric radial polymers wherein the different polymeric arms are contacted sequentially with a coupling agent. The method narrows the relative arm distribution of the several asymmetric radial polymers produced and significantly increases the amount of total product having the desired ratio of polymeric arms. Any coupling agent known in the prior art to be useful in the production of asymmetric radial polymers may be used in the method of this invention but coupling agents having from three to about twelve functional groups are most effective.