Thermoset interleafed resin matrix composites with improved compression properties

Claim 2

A reinforced interleafed filament resin matrix composite comprised of: (A) a fiber resin matrix composition; (B) an interleaf sheet formed of a heat-curable resin containing elastomeric material and having a polymer composition chemically compatible with the resin of the fiber resin matrix composition to form a cross-linked interface at the boundary between the fiber resin and the interleaf sheet and a discrete elastomeric layer.

Claim 3

A reinforced interleafed filament resin matrix composite as in Claim 1 wherein the elastomeric content of the interleafing sheet is above about 8 per cent.

Claim 4

A reinforced interleaf filament resin matrix composite as in Claim 1 wherein the viscosity of the interleaf measures an N number less than 14.6 when measured by the Flow (Viscosity) Test.

Claim 5

A reinforced interleaf filament resin matrix composite as in Claim 1 wherein the viscosity of the interleaf measures an N number less than 12 when measured by the Flow (Viscosity) Test.

Claim 6

A reinforced interleaf filament resin matrix composite as in Claim 1 wherein the viscosity measures an N number less than 7.7 when measured by the Flow (Viscosity) Test.

Claim 7

A reinforced interleafed filament resin matrix composite as in Claim 1 wherein the fiber resin matrix composition component (A) is comprised of: (i) reinforcing filaments; and (ii) a heat-curable resin in which the reinforcing filaments are imbedded.

Claim 8

A reinforced interleafed filament resin matrix composite as in Claim 6 wherein component (ii) is comprised of an epoxy resin prepolymer.

Claim 9

An interleafed fiber resin matrix composite which comprises: (A) A fiber resin matrix layer comprising (i) high-strength reinforcing filaments and (ii) a thermosetting epoxy resin composition coating said filaments, and (B) A discrete interleaf resin layer comprising (i) a thermosetting epoxy resin composition containing (ii) 8% to 70% by weight of a rubbery vinyl addition polymer, wherein said epoxy resin composition (A)(ii) exhibits shear modulus of at least 90,000 psi at high temperatures or at least 50,000 psi at high temperatures under wet conditions, and said interleaf resin (B) exhibits shear modulus of at least 50,000 psi and a yield strength of at least 3000 psi at high temperatures, and shear strain to failure of at least 6% at -67°F and at least 15% at room temperature.

Claim 10

An interleafed fiber resin matrix composite which comprises: (A) A fiber resin matrix layer comprising (i) high-strength reinforcing filaments and (ii) a thermosetting epoxy resin composition coating said filaments, and (B) A discrete interleaf resin layer comprising (i) a thermosetting epoxy resin composition containing (ii) 8% to 70% by weight of a rubbery vinyl addition polymer, wherein said epoxy resin composition (A)(ii) exhibits shear modulus of at least 90,000 psi at high temperatures or at least 50,000 psi at high temperatures under wet conditions, and said interleaf resin (B) exhibits shear modulus of at least 50,000 psi and a yield strength of at least 3000 psi at high temperatures, and shear strain to failure of at least 6% at -67°F and at least 15% at room temperature.

Claim 11

An interleafed fiber resin matrix composite comprising: (A) a fiber resin matrix comprising: (i) 60%-70% by weight high-strength reinforcing filaments selected from the group consisting of carbon fibers, graphite fibers, nickel-coated such fibers, silver-coated such fibers, nickel and-silver-coated such fibers, and combinations thereof, and (ii) 30%-40% by weight of a thermosetting epoxy resin composition coating said filaments, said epoxy resin composition comprising: (a) a polyepoxide compound or combination of compounds, (b) a curing agent effective to catalyze polymerization of said polyepoxide compound, and (c) a filler; and (B) a discrete interleaf resin layer comprising: (i) 40%-70% by weight a prereact comprising: (a) a conjugated diene elastomer, (b) a polyepoxide compound or combination of polyepoxide compounds, and (c) a curing agent effective to catalyze polymerization of said polyepoxide compound, in intimate admixture with (ii) 60%-30% by weight of a thermosetting epoxy resin composition comprising (a) a polyepoxide compound or a combination of polyepoxide compounds, wherein said poly-epoxide compound or combination (B)(ii)(a) is not the same compound or combination as that of the prereact component (B)(i)(b), (b) a curing agent effective to catalyze polymerization of said polyepoxide compound, and (c) a conjugated diene elastomer; wherein said epoxy resin composition (A)(ii) exhibits shear modulus of at least 50,000 psi at high temperatures under wet condiditions, and said interleaf resin (B) exhibits shear modulus of at least 50,000 psi and a yield strength of at least 3000 psi at high temperatures, and shear strain to failure of at least 6% at -67°F, at least 15% at room temperature and at least 25% at high temperatures.

Claim 12

An interleafed fiber resin matrix composite comprising: (A) a fiber resin matrix comprising: (i) 60%-70% by weight high-strength reinforcing filaments selected from the group consisting of carbon fibers, graphite fibers, nickel-coated such fibers, silver-coated such fibers, nickel and-silver-coated such fibers, and combinations thereof, and (ii) 30%-40% by weight of a thermosetting epoxy resin composition coating said filaments, said epoxy resin composition comprising: (a) a polyepoxide compound or combination of compounds, (b) a curing agent effective to catalyze polymerization of said polyepoxide compound, and (c) a filler; and (B) a discrete interleaf resin layer comprising: (i) 40%-70% by weight a prereact comprising: (a) a conjugated diene elastomer, (b) a polyepoxide compound or combination of polyepoxide compounds, and (c) a curing agent effective to catalyze polymerization of said polyepoxide compound, in intimate admixture with (ii) 60%-30% by weight of a thermosetting epoxy resin composition comprising (a) a polyepoxide compound or a combination of polyepoxide compounds, wherein said poly-epoxide compound or combination (B)(ii)(a) is not the same compound or combination as that of the prereact component (B)(i)(b), (b) a curing agent effective to catalyze polymerization of said polyepoxide compound, and (c) a conjugated diene elastomer; wherein said epoxy resin composition (A)(ii) exhibits shear modulus of at least 50,000 psi at high temperatures under wet condiditions, and said interleaf resin (B) exhibits shear modulus of at least 50,000 psi and a yield strength of at least 3000 psi at high temperatures, and shear strain to failure of at least 6% at -67°F, at least 15% at room temperature and at least 25% at high temperatures.

Claim 13

An interleafed fiber resin matrix composite comprising: (A) A fiber resin matrix layer comprising: (i) 60%-70% by weight high-strength reinforcing filaments selected from the group consisting of carbon fibers, graphite fibers, nickel-coated such fibers, silver-coated such fibers and nickel-and silver-coated such fibers, and (ii) 30%-40% by weight of a thermosetting epoxy resin composition coating said filaments, said epoxy resin composition comprising: (a) 50-100 parts by weight of tetra (4,4')N-glycidyl methylene dianiline, (b) 0-50 parts by weight tetra-glycidoxy tetraphenylethane, (c) 28-60 parts by weight trimethylene glycol di-para-aminobenzoate, (d) 0-12 parts by weight fumed silica, and (e) 0.1-2.5 parts by weight of the reaction product of toluene diisocyanate and dimethylamine; and (B) A discrete interleaf resin layer comprising (i) 40%-60% by weight of a prereact comprising: (a) 6-18 parts by weight of a carboxylic-functional butadiene-acrylonitrile copolymer, (b) 0-130 parts by weight of a diglycidyl ether of tetrabromo bisphenol A, (c) 0-130 parts by weight of a diglycidyl ether of bisphenol A, (d) 1-6 parts by weight of bisphenol A, (e) 0.05-0.25 parts by weight of triphenyl phosphine, and (f) 2-12 parts by weight of diaminodiphenyl sulphone, in intimate admixture with (ii) 40%-60% by weight of a thermosetting epoxy resin composition comprising: (a) 25-50 parts by weight of tetra (4,4')N-glycidyl methylene dianiline, (b) 10-30 parts by weight diaminodiphenyl sulfone, (c) 2-12 parts by weight of dicyandiamide, (d) 6-18 parts by weight of a carboxylic-functional butadiene-acrylonitrile copolymer, and (e) 0.5-1.5 parts by weight of titanium dioxide.

Claim 14

An interleafed fiber resin matrix composite comprising: (A) A fiber resin matrix layer comprising: (i) 60%-70% by weight high-strength reinforcing filaments selected from the group consisting of carbon fibers, graphite fibers, nickel-coated such fibers, silver-coated such fibers and nickel-and silver-coated such fibers, and (ii) 30%-40% by weight of a thermosetting epoxy resin composition coating said filaments, said epoxy resin composition comprising: (a) 50-100 parts by weight of tetra (4,4')N-glycidyl methylene dianiline, (b) 0-50 parts by weight tetra-glycidoxy tetraphenylethane, (c) 28-60 parts by weight trimethylene glycol di-para-aminobenzoate, (d) 0-12 parts by weight fumed silica, and (e) 0.1-2.5 parts by weight of the reaction product of toluene diisocyanate and dimethylamine; and (B) A discrete interleaf resin layer comprising (i) 40%-60% by weight of a prereact comprising: (a) 6-18 parts by weight of a carboxylic-functional butadiene-acrylonitrile copolymer, (b) 0-130 parts by weight of a diglycidyl ether of tetrabromo bisphenol A, (c) 0-130 parts by weight of a diglycidyl ether of bisphenol A, (d) 1-6 parts by weight of bisphenol A, (e) 0.05-0.25 parts by weight of triphenyl phosphine, and (f) 2-12 parts by weight of diaminodiphenyl sulphone, in intimate admixture with (ii) 40%-60% by weight of a thermosetting epoxy resin composition comprising: (a) 25-50 parts by weight of tetra (4,4')N-glycidyl methylene dianiline, (b) 10-30 parts by weight diaminodiphenyl sulfone, (c) 2-12 parts by weight of dicyandiamide, (d) 6-18 parts by weight of a carboxylic-functional butadiene-acrylonitrile copolymer, and (e) 0.5-1.5 parts by weight of titanium dioxide.

Claim 15

An interleafed fiber resin matrix composite which comprises: (A) A fiber resin matrix layer comprising (i) 60%-70% by weight high-strength reinforcing filaments and (ii) 30%-40% by weight of a thermosetting epoxy resin composition coating said filaments, and (B) A discrete interleaf resin layer comprising (i) a thermosetting epoxy resin composition containing (ii) 8% to 70% by weight of a rubbery vinyl addition polymer, wherein said thermosetting epoxy resin composition (A)(ii), subjected to shear forces at 200°F, has an ultimate stress of at least 5000 psi, and wherein said interleaf resin (B), subjected to shear at 200°F has a yield stress of at least 4000 psi, an ultimate stress of at least 5000 psi, and strain to failure of at least 15%, and wherein the shear modulus for epoxy resin composition (A)(ii) is at least 100,000 psi, and the shear modulus for interleaf resin (B) below the yield point is at least 100,000 psi.

Claim 16

An interleafed fiber resin matrix composite which comprises: (A) A fiber resin matrix layer comprising (i) 60%-70% by weight high-strength reinforcing filaments and (ii) 30%-40% by weight of a thermosetting epoxy resin composition coating said filaments, and (B) A discrete interleaf resin layer comprising (i) a thermosetting epoxy resin composition containing (ii) 8% to 70% by weight of a rubbery vinyl addition polymer, wherein said thermosetting epoxy resin composition (A)(ii), subjected to shear forces at 200°F, has an ultimate stress of at least 5000 psi, and wherein said interleaf resin (B), subjected to shear at 200°F has a yield stress of at least 4000 psi, an ultimate stress of at least 5000 psi, and strain to failure of at least 15%, and wherein the shear modulus for epoxy resin composition (A)(ii) is at least 100,000 psi, and the shear modulus for interleaf resin (B) below the yield point is at least 100,000 psi.

Claim 17

An interleafed fiber resin matrix composite which comprises: (A) A fiber resin matrix layer comprising (i) high-strength reinforcing filaments and (ii) a thermosetting epoxy resin composition coating said filaments, and (B) A discrete interleaf resin layer comprising (i) a thermosetting epoxy resin composition containing (ii) up to 70% by weight of a rubbery vinyl addition polymer, wherein the shear stress and shear strain properties of the thermosetting epoxy resin composition (A)(ii) and interleaf resin (B) are substantially as represented in Figure 5.

Claim 18

An interleafed fiber resin matrix composite which comprises: (A) A fiber resin matrix layer comprising (i) high-strength reinforcing filaments and (ii) a thermosetting epoxy resin composition coating said filaments, and (B) A discrete interleaf resin layer comprising (i) a thermosetting epoxy resin composition containing (ii) up to 70% by weight of a rubbery vinyl addition polymer, wherein the shear stress and shear strain properties of the thermosetting epoxy resin composition (A)(ii) and interleaf resin (B) are substantially as represented in Figure 5.

Claim 19

A process for producing an interleafed filament resin matrix comprising the steps of: (i) forming a fiber resin matrix composition; (ii) forming an interleaf cross-linked resin interface layer at the surface of the fiber resin matrix; and (iii) forming a discrete interleaf layer of polymer containing elastomer adjacent the interface layer.

Claim 20

A process for producing an interleafed filament resin matrix comprising the steps of: (i) forming a fiber resin matrix composition; (ii) forming an interleaf cross-linked resin interface layer at the surface of the fiber resin matrix; and (iii) forming a discrete interleaf layer of polymer containing elastomer adjacent the interface layer.

Claim 21

A process as in Claim 13 wherein the viscosity of the interleaf material measures an N number of 12 or less when measured by the Flow (Viscosity) Test.

Claim 22

A process as in Claim 13 wherein the interleaf material is at a viscosity which measures an N number of 7.7 or less when measured by the Flow (Viscosity) Test.