einforced polyamides and process of preparation thereof

Claim 2

A REINFORCED POLYMERIC COMPOSITION COMPRISING A AMIDE AND AT LEAST ABOUT 25% BY VOLUME OF AN INORGANIC FILLER MATERIAL HAVING A LENGTH TO DIAMETER RATIO OF UP TO ABOUT 25 TO 1, SAID MATERIAL HAVING BEEN TREATED WITH AN ORGANOSILANE COUPLING AGENT OF THE FORMULA

Claim 3

A reinforced polymeric composition according to claim 1 wherein said polyamide is a polylactam.

Claim 4

A reinforced polymeric composition according to claim 1 wherein said polyamide is a polylactam whose monomeric units contained at least six carbon atoms.

Claim 5

A reinforced polymeric composition according to claim 1 wherein said polyamide is polycaprolactam.

Claim 6

A reinforced polymeric composition according to claim 1 wherein siad polyamide is a condensation product of a polyamine and polycarboxylic acid.

Claim 7

A reinforced polymeric composition according to claim 1 wherein said polyamide is polyhexamethylene adipamide.

Claim 8

A reinforced polymeric composition according to claim 1 wherein said filler comprises from about 25 to about 90% by volume of the total composition.

Claim 9

A reinforced polymeric composition according to claim 1 wherein said filler comprises from about 33 to about 67% by volume of the total composition.

Claim 10

A reinforced polymeric composition according to claim 1 wherein said filler is an inorganic siliceous material which has a 3-dimensional crystal structure, a somewhat refractory nature with a melting point above about 800*C, a Mohs'' hardness of at least 4, and a water solubility of less than 0.1 gram per liter.

Claim 11

A reinforced polymeric composition according to claim 1 wherein said filler is a plate-like filler with a length to diameter ratio of less than 1 to 1.

Claim 12

A reinforced polymeric composition according to claim 1 wherein said filler has a length to diameter ratio from about 1 to 1 up to about 20 to 1.

Claim 13

A reinforced polymeric composition according to claim 1 wherein said coupling agent has the formula X3-Si-RnZ where X is halogen or alkoxy, R is an alkylene group having from about 2 to about 18 carbon atoms, Z is amino, secondary amido, isocyanato, halogen, alkoxycarbonyl, epoxy, vinyl, acryloxy, or methacryloxy, and n is 0 or 1, provided that n can be zero only when Z is a vinyl group.

Claim 14

A reinforced polymeric composition according to claim 1 wherein said coupling agent is 3-trialkoxysilylpropyl amine.

Claim 15

A reinforced polymeric composition according to claim 1 wherein said coupling agent is 11-(trialkoxysilyl)-undecyl bromide.

Claim 16

A reinforced polymeric composition according to claim 1 wherein said coupling agent is tri( Beta -methoxyethoxy)vinyl silane.

Claim 17

A reinforced polymeric composition according to claim 1 wherein said coupling agent is 3-(trialkoxysilyl)propyl chloride.

Claim 18

A reinforced polymeric composition according to claim 1 wherein said composition is characterized by a Strength Index at least triple that of an equivalently filled but uncoupled composition and a flexural modulus at least double that of the base resin.

Claim 19

A reinforced polymeric composition according to claim 1 wherein said polyamide is polycaprolactam or polyhexamethylene adipamide and wherein said composition is characterized by a Strength Index of at least 40 X 106 and a flexural modulus of at least 250,000 p.s.i.

Claim 20

A reinforced polymeric composition comprising a polyamide and from about 33 to about 67% by volume of an inorganic siliceous filler material which has a 3-dimensional crystal structure, a somewhat refractory nature with a melting point above about 800*C, a Mohs'' hardness of at least 4, a water solubility of less than 0.1 gram per liter and a length to diameter ratio from about 1 to 1 up to about 20 to 1, said filler material having been treated with an organosilane coupling agent of the formula X3-Si-RnZ where X is halogen or alkoxy, R is an alkylene group having from about 2 to about 18 carbon atoms, Z is amino, secondary amido, isocyanato, halogen, alkoxycarbonyl, cyclohexylepoxy, epoxy, vinyl acryloxy, or methacryloxy, and n is 0 to 1, provided that n can be zero only when Z is a vinyl group, said reinforced polymeric composition being characterized by a Strength Index at least triple that of an equivalently filled but uncoupled composition and a flexural modulus at least double that of the base resin.

Claim 21

A reinforced polymeric composition comprising a polyamide and from about 33 to about 67% by volume of an inorganic siliceous filler material which has a 3-dimensional crystal structure, a somewhat refractory nature with a melting point above about 800*C, a Mohs'' hardness of at least 4, a water solubility of less than 0.1 gram per liter and a length to diameter ratio from about 1 to 1 up to about 20 to 1, said filler material having been treated with an organosilane coupling agent of the formula X3-Si-RnZ where X is halogen or alkoxy, R is an alkylene group having from about 2 to about 18 carbon atoms, Z is amino, secondary amido, isocyanato, halogen, alkoxycarbonyl, cyclohexylepoxy, epoxy, vinyl acryloxy, or methacryloxy, and n is 0 to 1, provided that n can be zero only when Z is a vinyl group, said reinforced polymeric composition being characterized by a Strength Index at least triple that of an equivalently filled but uncoupled composition and a flexural modulus at least double that of the base resin.

Claim 22

A reinforced polymeric composition according to claim 19 wherein said polyamide is polycaprolactam or polyhexamethylene adipamide and wherein said composition is characterized by a Strength Index of at least 40 X 106 and a flexural modulus of at least 250,000.

Claim 23

A process for preparing a filler-reinforced polyamide composition having at least 25% by volume filler comprising (a) treating an inorganic filler material having a length to diameter ratio of at least 1 to 1 up to about 25 to 1 with an organosilane coupling agent of the formula

Claim 24

A process for preparing a filler-reinforced polyamide composition having at least 25% by volume filler comprising (a) treating an inorganic filler material having a length to diameter ratio of at least 1 to 1 up to about 25 to 1 with an organosilane coupling agent of the formula

Claim 25

A process according to claim 21 wherein said filler is treated with said coupler prior to its addition to the monomer.

Claim 26

A process according to claim 21 wherein the monomer which is polymerized is epsilon -caprolactam.

Claim 27

A process according to claim 21 wherein the Z group of said organosilane coupling agent is an amino group having at least one hydrogen atom, which amino group functions as a polymerization regulator.

Claim 28

A process according to claim 21 wherein said organosilane coupling agent has the formula (R1O)3Si-R-NH2 where R1 is an alkyl group and R is an alkylene group having from about 2 to 18 carbon atoms.

Claim 29

A process according to claim 21 wherein said organosilane coupling agent is 3-(triethoxysilyl)propyl amine.

Claim 30

A process according to claim 21 wherein the Z group of said organosilane coupling agent contains a nitrogen atom capable of functioning as a polymerization promoter.

Claim 31

A process according to claim 21 wherein said organosilane coupling agent is N-phenyl, N''-3-(triethoxysilyl)propyl urea.

Claim 32

A process according to claim 21 wherein the promoter is a polyfunctional isocyanate.

Claim 33

A process according to claim 21 wherein the catalyst is an alkylmagnesium halide.

Claim 34

A process according to claim 21 wherein the catalyst is sodium caprolactam.

Claim 35

A process according to claim 21 wherein said filler is an inorganic siliceous material having a length to diameter ratio of from about 1 to 1 up to about 25 to 1, a three-dimensional crystal structure, a somewhat refractory nature with a melting point above about 800*C, a Mohs'' hardness of at least 4, and a water solubility of less than 0.1 gram per liter.

Claim 36

A process for preparing a filler-reinforced polyamide composition having at least 25% by volume filler comprising (a) adding to a monomeric lactam, an inorganic siliceous filler having a length to diameter ratio of at least up to about 25 to 1, a somewhat refractory nature with a melting point above about 800*C, a Mohs'' hardness of at least 4, and a water solubility of less than 0.1 gram per liter, an organosilane coupling agent of the formula (R1O)3-Si-R-NH2 where R1 is an alkyl group and R is an alkylene group having from about 2 to 18 carbon atoms, and a lactam polymerization promoter, (b) removing volatile reaction products if any, (c) holding the umpolymerized mixture for an indefinite period of time. (d) adding a lactam polymerization catalyst, (e) casing the resultant mixture into a mold, and (f) maintaining the mixture at a temperture and for a time sufficient to achieve polymerization.

Claim 37

A process for preparing a filler-reinforced polyamide composition having at least 25% by volume filler comprising (a) adding to a monomeric lactam, an inorganic siliceous filler having a length to diameter ratio of at least up to about 25 to 1, a somewhat refractory nature with a melting point above about 800*C, a Mohs'' hardness of at least 4, and a water solubility of less than 0.1 gram per liter, an organosilane coupling agent of the formula (R1O)3-Si-R-NH2 where R1 is an alkyl group and R is an alkylene group having from about 2 to 18 carbon atoms, and a lactam polymerization promoter, (b) removing volatile reaction products if any, (c) holding the umpolymerized mixture for an indefinite period of time. (d) adding a lactam polymerization catalyst, (e) casing the resultant mixture into a mold, and (f) maintaining the mixture at a temperture and for a time sufficient to achieve polymerization.

Claim 38

A reinforced polyamide article comprising a polyamide and at least 25% by volume of an inorganic filler material having a length to diameter ratio of up to about 25 to 1 and a water solubility of less than 0.15 grams per liter, said material having been treated with an organosilane coupling agent of the formula

Claim 39

A reinforced polyamide article comprising a polyamide and at least 25% by volume of an inorganic filler material having a length to diameter ratio of up to about 25 to 1 and a water solubility of less than 0.15 grams per liter, said material having been treated with an organosilane coupling agent of the formula

Claim 40

A reinforced polyamide article according to claim 34, said article characterized by a Strength Index at least triple that of an equivalently filled but uncoupled article and a flexural modulus at least double that of an unfilled article made from the base polyamide resin.

Claim 41

A reinforced polymeric composition according to claim 17 wherein said polyamide is a polylactam.

Claim 42

A reinforced polymeric composition according to claim 17 wherein said polyamide is a condensation product of a polyamine and a polycarboxylic acid.

Claim 43

A reinforced polymeric composition according to claim 1 wherein said filler is a crystalline silica having a maximum particle size of about 5 microns and an average particle size of about 2 microns.

Claim 44

A reinforced polymeric composition according to claim 1 wherein said coupling agent has the formula X3-Si-R-Z where X is halogen or alkoxy, R is an alkylene group having from about 2 to 18 carbon atoms, and Z is amino, secondary amido, isocyanato, alkoxycarbonyl or epoxy.

Claim 45

A reinforced polymeric composition comprising a polyamide and from about 33 to 67% by volume of an inorganic siliceous filler material which is characterized by a 3-dimensional crystal structure, a somewhat refractory nature with a melting point above about 800*C, a Mohs'' hardness of at least 4, a water solubility of less than about 0.1 gram per liter and a length to diameter ratio from about 1:1 up to about 20:1, said filler material having been treated with an organosilane coupling agent of the formula X3-Si-R-Z where X is halogen or alkoxy, R is an alkylene group having from about 2 to 18 carbon atoms, and Z is amino, secondary amido, isocyanato, alkoxycarbonyl or epoxy, said reinforced polymeric composition being characterized by a Strength Index at least triple that of an equivalently filled but uncoupled composition and a flexural modulus at least double that of the base resin.

Claim 46

A reinforced polymeric composition comprising a polyamide and from about 33 to 67% by volume of an inorganic siliceous filler material which is characterized by a 3-dimensional crystal structure, a somewhat refractory nature with a melting point above about 800*C, a Mohs'' hardness of at least 4, a water solubility of less than about 0.1 gram per liter and a length to diameter ratio from about 1:1 up to about 20:1, said filler material having been treated with an organosilane coupling agent of the formula X3-Si-R-Z where X is halogen or alkoxy, R is an alkylene group having from about 2 to 18 carbon atoms, and Z is amino, secondary amido, isocyanato, alkoxycarbonyl or epoxy, said reinforced polymeric composition being characterized by a Strength Index at least triple that of an equivalently filled but uncoupled composition and a flexural modulus at least double that of the base resin.

Claim 47

A reinforced polymeric composition according to claim 1 wherein said filler has a Mohs'' hardness of at least 4.

Claim 48

A reinforced polymeric composition according to claim 41 wherein said filler has been treated with an organosilane coupling agent having the formula X3-Si-R-Z where X is alkoxy having up to 8 carbon atoms, R is an alkylene group having from about 2 to about 18 carbon atoms and Z is amino.

Claim 49

A reinforced polymeric composition according to claim 42 wherein said coupling agent is 3-triethoxysilylpropyl amine.

Claim 50

A reinforced polymeric composition according to claim 43 wherein the polyamide is polycaprolactam.

Claim 51

A reinforced polymeric composition according to claim 43 wherein the polyamide is polyhexamethylene adipamide.