US20200047430A1 - Fiber-reinforced resin molding material and method for manufacturing same, and fiber-reinforced resin molded article - Google Patents

Fiber-reinforced resin molding material and method for manufacturing same, and fiber-reinforced resin molded article Download PDF

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Publication number
US20200047430A1
US20200047430A1 US16/655,841 US201916655841A US2020047430A1 US 20200047430 A1 US20200047430 A1 US 20200047430A1 US 201916655841 A US201916655841 A US 201916655841A US 2020047430 A1 US2020047430 A1 US 2020047430A1
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Prior art keywords
fiber
reinforced resin
molding material
resin molding
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US16/655,841
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English (en)
Inventor
Yukichi Konami
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Mitsubishi Chemical Corp
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Mitsubishi Chemical Corp
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Assigned to MITSUBISHI CHEMICAL CORPORATION reassignment MITSUBISHI CHEMICAL CORPORATION ASSIGNMENT OF ASSIGNORS INTEREST (SEE DOCUMENT FOR DETAILS). Assignors: KONAMI, YUKICHI
Publication of US20200047430A1 publication Critical patent/US20200047430A1/en
Priority to US17/368,889 priority Critical patent/US12269221B2/en
Abandoned legal-status Critical Current

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    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
    • B29C—SHAPING OR JOINING OF PLASTICS; SHAPING OF MATERIAL IN A PLASTIC STATE, NOT OTHERWISE PROVIDED FOR; AFTER-TREATMENT OF THE SHAPED PRODUCTS, e.g. REPAIRING
    • B29C70/00—Shaping composites, i.e. plastics material comprising reinforcements, fillers or preformed parts, e.g. inserts
    • B29C70/04—Shaping composites, i.e. plastics material comprising reinforcements, fillers or preformed parts, e.g. inserts comprising reinforcements only, e.g. self-reinforcing plastics
    • B29C70/06—Fibrous reinforcements only
    • B29C70/10—Fibrous reinforcements only characterised by the structure of fibrous reinforcements, e.g. hollow fibres
    • B29C70/16—Fibrous reinforcements only characterised by the structure of fibrous reinforcements, e.g. hollow fibres using fibres of substantial or continuous length
    • B29C70/20—Fibrous reinforcements only characterised by the structure of fibrous reinforcements, e.g. hollow fibres using fibres of substantial or continuous length oriented in a single direction, e.g. roofing or other parallel fibres
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
    • B29B—PREPARATION OR PRETREATMENT OF THE MATERIAL TO BE SHAPED; MAKING GRANULES OR PREFORMS; RECOVERY OF PLASTICS OR OTHER CONSTITUENTS OF WASTE MATERIAL CONTAINING PLASTICS
    • B29B15/00—Pretreatment of the material to be shaped, not covered by groups B29B7/00 - B29B13/00
    • B29B15/08—Pretreatment of the material to be shaped, not covered by groups B29B7/00 - B29B13/00 of reinforcements or fillers
    • B29B15/10—Coating or impregnating independently of the moulding or shaping step
    • B29B15/12—Coating or impregnating independently of the moulding or shaping step of reinforcements of indefinite length
    • B29B15/122—Coating or impregnating independently of the moulding or shaping step of reinforcements of indefinite length with a matrix in liquid form, e.g. as melt, solution or latex
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
    • B29C—SHAPING OR JOINING OF PLASTICS; SHAPING OF MATERIAL IN A PLASTIC STATE, NOT OTHERWISE PROVIDED FOR; AFTER-TREATMENT OF THE SHAPED PRODUCTS, e.g. REPAIRING
    • B29C70/00—Shaping composites, i.e. plastics material comprising reinforcements, fillers or preformed parts, e.g. inserts
    • B29C70/04—Shaping composites, i.e. plastics material comprising reinforcements, fillers or preformed parts, e.g. inserts comprising reinforcements only, e.g. self-reinforcing plastics
    • B29C70/06—Fibrous reinforcements only
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
    • B29C—SHAPING OR JOINING OF PLASTICS; SHAPING OF MATERIAL IN A PLASTIC STATE, NOT OTHERWISE PROVIDED FOR; AFTER-TREATMENT OF THE SHAPED PRODUCTS, e.g. REPAIRING
    • B29C70/00—Shaping composites, i.e. plastics material comprising reinforcements, fillers or preformed parts, e.g. inserts
    • B29C70/04—Shaping composites, i.e. plastics material comprising reinforcements, fillers or preformed parts, e.g. inserts comprising reinforcements only, e.g. self-reinforcing plastics
    • B29C70/06—Fibrous reinforcements only
    • B29C70/10—Fibrous reinforcements only characterised by the structure of fibrous reinforcements, e.g. hollow fibres
    • B29C70/16—Fibrous reinforcements only characterised by the structure of fibrous reinforcements, e.g. hollow fibres using fibres of substantial or continuous length
    • B29C70/22—Fibrous reinforcements only characterised by the structure of fibrous reinforcements, e.g. hollow fibres using fibres of substantial or continuous length oriented in at least two directions forming a two-dimensional [2D] structure
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
    • B29K—INDEXING SCHEME ASSOCIATED WITH SUBCLASSES B29B, B29C OR B29D, RELATING TO MOULDING MATERIALS OR TO MATERIALS FOR MOULDS, REINFORCEMENTS, FILLERS OR PREFORMED PARTS, e.g. INSERTS
    • B29K2031/00—Use of polyvinylesters or derivatives thereof as moulding material
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
    • B29K—INDEXING SCHEME ASSOCIATED WITH SUBCLASSES B29B, B29C OR B29D, RELATING TO MOULDING MATERIALS OR TO MATERIALS FOR MOULDS, REINFORCEMENTS, FILLERS OR PREFORMED PARTS, e.g. INSERTS
    • B29K2307/00—Use of elements other than metals as reinforcement
    • B29K2307/04—Carbon

Definitions

  • the present invention relates to a fiber-reinforced resin molding material and a method for manufacturing thereof, and a fiber-reinforced resin molded article.
  • fiber-reinforced resin molded articles are widely used since these are lightweight and have a high strength.
  • a prepreg in which a reinforcement fiber sheet formed of continuous fibers (long fibers) formed of reinforcement fibers is impregnated with a resin composition is widely used.
  • a plurality of prepregs are laminated in a press tool, and then heated and pressed by the press tool to obtain a fiber-reinforced resin molded article.
  • a thermosetting resin composition is used as a resin composition in a prepreg, and an epoxy resin composition is frequently used in view of good mechanical properties (Patent Literatures 1 and 2).
  • An object of the invention is to provide a fiber-reinforced resin molding material with which a lightweight and high-strength fiber-reinforced resin molded article can be easily obtained and a method for manufacturing the fiber-reinforced resin molding material, and a fiber-reinforced resin molded article using the fiber-reinforced resin molding material.
  • the invention has the following configuration.
  • a fiber-reinforced resin molding material including: a reinforcement fiber sheet whose basis weight is 200 g/m 2 or greater and 3,000 g/m 2 or less; and a resin composition which is impregnated into the reinforcement fiber sheet such that a content of the resin composition is 25 volume % or greater and 55 volume % or less, in which in a case where a total amount of the resin composition contained in the fiber-reinforced resin molding material is 100 mass %, a thickness from a first surface in a thickness direction of the fiber-reinforced resin molding material to a position occupied by 10 mass % of the resin composition is represented by d1 ( ⁇ m), and a thickness from a second surface opposite to the first surface to a position occupied by 10 mass % of the resin composition is represented by d2 ( ⁇ m), an absolute value (
  • the reinforcement fiber sheet is formed of at least one selected from the group consisting of a unidirectional sheet in which a plurality of continuous fibers are arranged in parallel in one direction, a woven fabric in which continuous fibers are woven, and a non-crimp fabric containing continuous fibers.
  • a method for manufacturing a fiber-reinforced resin molding material including: impregnating a reinforcement fiber sheet formed of at least one selected from the group consisting of a unidirectional sheet in which a plurality of continuous fibers are arranged in parallel in one direction, a woven fabric in which continuous fibers are woven, and a non-crimp fabric containing continuous fibers with a resin composition having an initial viscosity of 1 Pa ⁇ s or less and having a viscosity of 5,000 Pa ⁇ s or greater and 150,000 Pa ⁇ s or less after leaving for 7 days at 25° C.
  • a fiber-reinforced resin molding material with which a lightweight and high-strength fiber-reinforced resin molded article can be easily obtained can be manufactured.
  • the fiber-reinforced resin molded article according to the invention can be easily manufactured. In addition, it is lightweight and has a high strength.
  • FIG. 1 is a schematic configuration diagram showing an example of a manufacturing apparatus used for manufacturing a fiber-reinforced resin molding material according to the invention.
  • a reinforcement fiber sheet is impregnated with a resin composition.
  • the reinforcement fiber sheet is at least one selected from the group consisting of a unidirectional sheet (UD sheet) in which a plurality of continuous fibers are arranged in parallel in one direction, a woven fabric (cloth material) in which continuous fibers are woven, and a non-crimp fabric (NCF) containing continuous fibers.
  • UD sheet unidirectional sheet
  • cloth material cloth material
  • NCF non-crimp fabric
  • the continuous fiber means a reinforcement fiber that is continuous over a length of 75 mm or longer, preferably 500,000 mm or shorter, and more preferably 100 mm or longer and 10,000 mm or shorter in at least one direction.
  • the upper limit of the range of the length may be a winding amount of carbon fiber, that is a raw material of the reinforcement fiber sheet, per one bobbin.
  • any one of a unidirectional sheet, a woven fabric, and a non-crimp fabric may be used alone, or two or more of a unidirectional sheet, a woven fabric, and a non-crimp fabric may be used in combination.
  • the reinforcement fiber sheet is preferably a woven fabric or a non-crimp fabric in view of strength.
  • a non-crimp fabric is more preferable since a reinforcement fiber composite molded article having excellent mechanical properties with small crimps of continuous fibers is obtained.
  • the weaving method for the woven fabric is not particularly limited, and examples thereof include plain weave, twill weave, satin weave, cord weave, and triaxial weave.
  • the non-crimp fabric is a sheet-like substrate in which a plurality of continuous fibers are integrated by auxiliary fiber yarn forming a warp-knitted structure without crossing each other.
  • a known aspect can be employed as the non-crimp fabric, and examples thereof include a form having one or more layers in which a plurality of continuous fibers are arranged in parallel in layers in one direction. In a case where the non-crimp fabric has two or more layers, fiber axis directions of the continuous fibers of the layers may be parallel to each other or may intersect.
  • the auxiliary fiber yarn is not particularly limited, and examples thereof include monofilament yarn or multifilament yarn made of polyester, polyamide, polyethylene, polylactic acid, or the like, aramid fibers, cotton yarn, and silk yarn.
  • the continuous fiber is not particularly limited, and examples thereof include inorganic fibers, organic fibers, metallic fibers, and reinforcement fibers having a hybrid structure obtained by combining the above fibers.
  • Examples of the inorganic fibers include carbon fibers, graphite fibers, silicon carbide fibers, alumina fibers, tungsten carbide fibers, boron fibers, and glass fibers.
  • Examples of the organic fibers include aramid fibers, high-density polyethylene fibers, other general nylon fibers, and polyester fibers.
  • Examples of the metallic fibers include stainless steel fibers and iron fibers. Metal-coated carbon fibers may also be included.
  • the continuous fibers may be used singly or in combination of two or more types thereof.
  • the average fiber diameter of the continuous fibers is preferably 1 ⁇ m or greater and 50 ⁇ m or less, and more preferably 5 ⁇ m or greater and 20 ⁇ m or less.
  • carbon fibers are preferable in view of mechanical properties such as a strength of a fiber-reinforced resin molded article.
  • the carbon fibers preferably have a strand tensile strength of 1.0 GPa or greater and 9.0 GPa or less, and more preferably 1.5 GPa or greater and 9.0 GPa or less, measured according to JIS R 7601: 1986.
  • the carbon fibers preferably have a strand tensile elastic modulus of 150 GPa or greater and 1,000 GPa or less, and more preferably 200 GPa or greater and 1,000 GPa or less, measured according to JIS R 7601: 1986.
  • the basis weight of the reinforcement fiber sheet is 200 g/m 2 or greater and 3,000 g/m 2 or less, preferably 300 g/m 2 or greater and 2,500 g/m 2 or less, and more preferably 400 g/m 2 or greater and 2,000 g/m 2 or less.
  • the basis weight of the reinforcement fiber sheet is 200 g/m 2 or greater, preferably 300 g/m 2 or greater, and more preferably 400 g/m 2 or greater, the number of reinforcement fiber sheets to be laminated can be reduced even in manufacturing of a fiber-reinforced resin molded article having a large thickness, and excellent workability is obtained. Accordingly, the fiber-reinforced resin molded article can be easily manufactured.
  • a high-strength fiber-reinforced resin molded article can be obtained, and the performance variation of the fiber-reinforced resin molded article to be obtained is also small.
  • the basis weight of the reinforcement fiber sheet is 3,000 g/m 2 or less, preferably 2,500 g/m 2 or less, and more preferably 2,000 g/m 2 or less, the impregnation properties of the resin composition into the reinforcement fiber sheet is excellent.
  • the content of the resin composition in the fiber-reinforced resin molding material according to the invention is 25 volume % or greater and 55 volume % or less, preferably 30 volume % or greater and 50 volume % or less, and more preferably 35 volume % or greater and 45 volume % or less with respect to the total volume of the fiber-reinforced resin molding material.
  • the content of the resin composition is 55 volume % or less, preferably 50 volume % or less, and more preferably 45 volume % or less, a lightweight fiber-reinforced resin molded article can be obtained.
  • the fiber-reinforced resin molded article has a high strength due to a relatively high proportion of the continuous fibers.
  • the fiber-reinforced resin molding material it is possible to suppress an excessive increase in tackiness of a surface of the fiber-reinforced resin molding material. Accordingly, for example, even in a case where a plurality of fiber-reinforced resin molding materials are misaligned when being laminated, and the fiber-reinforced resin molding materials laminated once are re-laminated, it is possible to suppress work difficulties caused by adhesion between the fiber-reinforced resin molding materials. In a case where the content of the resin composition is 25 volume % or greater, preferably 30 volume % or greater, and more preferably 35 volume % or greater, it is possible to suppress a deterioration in appearance of the fiber-reinforced resin molded article due to the occurrence of resin deficiency.
  • a thickness from a first surface in a thickness direction of the fiber-reinforced resin molding material to a position occupied by 10 mass % of the resin composition is represented by d1 ( ⁇ m)
  • a thickness from a second surface opposite to the first surface to a position occupied by 10 mass % of the resin composition is represented by d2 ( ⁇ m).
  • ) of the difference between d1 and d2 is 50 ⁇ m or less, preferably 20 ⁇ m or less, and more preferably 15 ⁇ m or less.
  • the absolute value of the difference between d1 and d2 is equal to or less than the upper limit value of the above range, an excessive increase in tackiness of a surface of the fiber-reinforced resin molding material is easily suppressed. Accordingly, for example, even in a case where a plurality of fiber-reinforced resin molding materials are misaligned when being laminated, and the fiber-reinforced resin molding materials laminated once are re-laminated, the fiber-reinforced resin molding materials are less likely to further adhere to each other, and the work is thus facilitated.
  • the sum of d1 and d2 is preferably 10 ⁇ m or greater and 1,500 ⁇ m or less.
  • the sum of d1 and d2 is more preferably 15 ⁇ m or greater and 1,200 ⁇ m or less, even more preferably 20 ⁇ m or greater and 1,000 ⁇ m or less, and particularly preferably 30 ⁇ m or greater and 800 ⁇ m or less.
  • the sum of d1 and d2 is 10 ⁇ m or greater, more preferably 15 ⁇ m or greater, even more preferably 20 ⁇ m or greater, and particularly preferably 30 ⁇ m or greater, an excessive increase in tackiness of the fiber-reinforced resin molding material is easily suppressed.
  • the fiber-reinforced resin molding materials are less likely to further adhere to each other, and the work is thus facilitated.
  • the sum of d1 and d2 is 1,500 ⁇ m or less, more preferably 1,200 ⁇ m or less, even more preferably 1,000 ⁇ m or less, and particularly preferably 800 ⁇ m or less, the fiber-reinforced resin molding material has sufficient tackiness, and thus the fiber-reinforced resin molding materials laminated are less likely to misalign.
  • the first surface in the thickness direction is a surface on the lower side (in the direction of gravity) in manufacturing of the fiber-reinforced resin molding material.
  • the first surface is in contact with a carrier film conveying portion 14 .
  • the second surface on the opposite side is a surface positioned on the opposite side to the first surface.
  • a ratio R ((d1+d2)/(basis weight)) of the sum ( ⁇ m) of d1 and d2 to the basis weight (g/m 2 ) of the reinforcement fiber sheet is preferably within a range of 0.2 or greater and 0.5 or less.
  • the ratio R is more preferably 0.2 or greater and 0.4 or less, and even more preferably 0.25 or greater and 0.3 or less.
  • the thickness d1 is preferably 5 ⁇ m or greater and 750 ⁇ m or less, more preferably 7 ⁇ m or greater and 600 ⁇ m or less, even more preferably 10 ⁇ m or greater and 500 ⁇ m or less, and particularly preferably 15 ⁇ m or greater and 400 ⁇ m or less.
  • the thickness d1 is 5 ⁇ m or greater, more preferably 7 ⁇ m or greater, even more preferably 10 ⁇ m or greater, and particularly preferably 15 ⁇ m or greater, an excessive increase in tackiness of the first surface of the fiber-reinforced resin molding material is easily suppressed.
  • the fiber-reinforced resin molding materials are less likely to further adhere to each other, and the work is thus facilitated.
  • the thickness d1 is 750 ⁇ m or less, more preferably 600 ⁇ m or less, even more preferably 500 ⁇ m or less, and particularly preferably 400 ⁇ m or less, the first surface of the fiber-reinforced resin molding material has sufficient tackiness, and thus the fiber-reinforced resin molding materials laminated are less likely to misalign.
  • a preferable range of the thickness d2 is preferably 5 ⁇ m or greater and 750 ⁇ m or less, more preferably 7 ⁇ m or greater and 600 ⁇ m or less, even more preferably 10 ⁇ m or greater and 500 ⁇ m or less, and particularly preferably 15 ⁇ m or greater and 400 ⁇ m or less in view of tackiness of the second surface as in the case of the thickness d1.
  • a fiber volume fraction (Vf) of the fiber-reinforced resin molding material according to the invention is preferably 45 volume % or greater and 75 volume % or less, more preferably 50 volume % or greater and 70 volume % or less, and even more preferably 55 volume % or greater and 65 volume % or less.
  • the fiber volume fraction (Vf) is 45 volume % or greater, more preferably 50 volume % or greater, and even more preferably 55 volume % or greater, a high-strength fiber-reinforced resin molded article is easily obtained.
  • Vf the fiber volume fraction (Vf) is 75 volume % or less, more preferably 70 volume % or less, and even more preferably 65 volume % or less, a fiber-reinforced resin molded article with excellent impregnation properties and appearance, in which resin deficiency is easily suppressed, is easily obtained.
  • the fiber volume fraction (Vf) is a value obtained by the measurement method according to JIS K7075.
  • the resin composition preferably contains a thermosetting resin.
  • the thermosetting resin include an epoxy resin, a vinyl ester resin, an unsaturated polyester resin, a polyimide resin, a maleimide resin, and a phenol resin.
  • the thermosetting resins may be used singly or in combination of two or more types thereof.
  • thermosetting resin is preferably an epoxy resin or a vinyl ester resin in view of adhesion to carbon fibers, and more preferably a vinyl ester resin in view of the fact that a fiber-reinforced resin molding material with which a lightweight and high-strength fiber-reinforced resin molded article can be easily manufactured is easily obtained.
  • the vinyl ester resin is preferably a resin obtained through an addition reaction of an epoxy compound having two or more epoxy groups in the molecule, a (meth)acrylic acid, and an optional polybasic acid or anhydride thereof.
  • the epoxy compound examples include epoxy resins such as bisphenol A epoxy resins, bisphenol F epoxy resins, hydrogenated bisphenol epoxy resins, phenol novolac epoxy resins, and cresol novolac epoxy resins; glycidyl ether of polyhydric alcohols such as neopentyl glycol diglycidyl ether, polypropylene glycol diglycidyl ether, and trimethylolpropane triglycidyl ether; and glycidyl ester of polybasic acids such as phthalic acid diglycidyl ester and dimer acid diglycidyl ester.
  • the epoxy compounds may be used singly or in combination of two or more types thereof.
  • polybasic acids or anhydrides thereof examples include ⁇ , ⁇ -unsaturated dibasic acids such as maleic acid, maleic anhydride, fumaric acid, and itaconic acid; saturated dibasic acids such as oxalic acid, malonic acid, and succinic acid; pyromellitic acid; trimellitic acid; trimer acid; polybutadiene having a carboxyl group; butadiene-acrylonitrile copolymers having a carboxyl group; and compounds having a carboxyl group at a terminal, obtained by esterification of ⁇ , ⁇ -unsaturated dibasic acid and/or saturated dibasic acid and polyhydric alcohols.
  • the polybasic acids or anhydrides thereof may be used singly or in combination of two or more types thereof.
  • the content of the thermosetting resin in the resin composition is preferably 30 volume % or greater and 50 volume % or less, and more preferably 35 volume % or greater and 45 volume % or less with respect to the total volume of the resin composition.
  • the content of the thermosetting resin is equal to or greater than the lower limit value of the above range, a high-strength fiber-reinforced resin molded article is easily obtained.
  • the content of the thermosetting resin is equal to or less than the upper limit value of the above range, a fiber-reinforced resin molded article with excellent impregnation properties and appearance, in which resin deficiency is easily suppressed, is easily obtained.
  • the resin composition may contain a thermoplastic resin such as a polyamide resin and a polyolefin resin.
  • the resin composition may contain additives such as a curing agent, a flame retardant, a weather resistance improver, an antioxidant, a heat stabilizer, an ultraviolet absorber, a plasticizer, a lubricant, a colorant, a compatibilizing agent, and a conductive filler according to properties required for the fiber-reinforced resin molded article.
  • additives such as a curing agent, a flame retardant, a weather resistance improver, an antioxidant, a heat stabilizer, an ultraviolet absorber, a plasticizer, a lubricant, a colorant, a compatibilizing agent, and a conductive filler according to properties required for the fiber-reinforced resin molded article.
  • curing agent known curing agents suitable for the resin composition to be used can be used.
  • a general organic peroxide is preferable in a case where a vinyl ester resin or an unsaturated polyester resin is used.
  • an epoxy resin is used, an amine-based or acid anhydride-based curing agent is preferable.
  • the above-described reinforcement fiber sheet formed of at least one selected from a unidirectional sheet, a woven fabric, and a non-crimp fabric, and having a basis weight of 200 g/m 2 or greater and 3,000 g/m 2 or less is impregnated with a resin composition such that the content of the resin composition is 25 volume % or greater and 55 volume % or less.
  • the reinforcement fiber sheet has a high basis weight so as to satisfy the above range, the number of fiber-reinforced resin molding materials to be laminated can be reduced even in manufacturing of a fiber-reinforced resin molded article having a large thickness.
  • the content of the resin composition is as small as to satisfy the above range, it is possible to suppress an excessive increase in tackiness of the surface of the fiber-reinforced resin molding material. Accordingly, for example, even in a case where a plurality of fiber-reinforced resin molding materials are misaligned when being laminated, and the fiber-reinforced resin molding materials laminated once are re-laminated, the fiber-reinforced resin molding materials are less likely to further adhere to each other, and the work is thus facilitated. Therefore, a fiber-reinforced resin molded article can be easily manufactured using the fiber-reinforced resin molding material according to the invention.
  • the content of the resin composition is small, the weight of the fiber-reinforced resin molded article can be reduced, and since the content of the continuous fibers is relatively large, a high-strength fiber-reinforced resin molded article can be obtained.
  • a method for manufacturing a fiber-reinforced resin molding material according to the invention is a method for manufacturing the above-described fiber-reinforced resin molding material according to the invention.
  • a fiber-reinforced resin molding material is obtained in which a reinforcement fiber sheet formed of at least one selected from the group consisting of a unidirectional sheet in which a plurality of continuous fibers are arranged in parallel in one direction, a woven fabric in which continuous fibers are woven, and a non-crimp fabric containing continuous fibers, and having a basis weight of 200 g/m 2 or greater and 3,000 g/m 2 or less is impregnated with a resin composition, and the content of the resin composition is 25 volume % or greater and 55 volume % or less.
  • a fiber-reinforced resin molding material manufacturing apparatus 100 illustrated in FIG. 1 (hereinafter, simply referred to as “manufacturing apparatus 100 ”) is used.
  • manufactured apparatus 100 an XYZ rectangular coordinate system is set, and positional relationships between members will be described with reference to the XYZ rectangular coordinate system as necessary.
  • the manufacturing apparatus 100 includes a reinforcement fiber sheet supply portion 10 , a first unwinder 12 , a carrier film conveying portion 14 , a first coating portion 16 , a second unwinder 18 , a second coating portion 20 , an impregnation portion 22 , and a winder 24 .
  • the first unwinder 12 is provided with a first raw sheet roll R 1 on which a long first carrier film C 1 is wound. A long first carrier film C 1 is unwound from the first raw sheet roll R 1 by the first unwinder 12 , and supplied to the carrier film conveying portion 14 .
  • the carrier film conveying portion 14 includes a conveyor 15 in which an endless belt 15 c is hung between a pair of pulleys 15 a and 15 b .
  • the endless belt 15 c is circulated by rotating the pair of pulleys 15 a and 15 b in the same direction, and the first carrier film C 1 is conveyed to the right in the X-axis direction on a surface of the endless belt 15 c .
  • a mesh belt can be used as the endless belt 15 c.
  • the first coating portion 16 is positioned immediately above the carrier film conveying portion 14 on the side of the pulley 15 a , and includes a doctor blade 17 which applies a resin composition P.
  • the resin composition P of a predetermined thickness is coated on a surface of the first carrier film C 1 by the doctor blade 17 , and a first resin sheet S 1 is formed.
  • the first resin sheet S 1 travels along with conveyance of the first carrier film C 1 .
  • the reinforcement fiber sheet supply portion 10 supplies a long reinforcement fiber sheet F.
  • a raw sheet roll R in which the reinforcement fiber sheet F is wound around a bobbin is rotatably held by a creel.
  • the reinforcement fiber sheet F supplied by the reinforcement fiber sheet supply portion 10 is continuously laminated on the first resin sheet S 1 traveling along with conveyance of the first carrier film C 1 by guide rolls 11 .
  • the second unwinder 18 is provided with a second raw sheet roll R 2 on which a long second carrier film C 2 is wound.
  • a long second carrier film C 2 is unwound from the second raw sheet roll R 2 , and by a plurality of guide rolls 19 , the long second carrier film is supplied to a downstream side of a position to which the reinforcement fiber sheet F on the carrier film conveying portion 14 is supplied.
  • the second carrier film C 2 unwound from the second unwinder 18 is conveyed in a direction (on the left side in the X-axis direction) opposite to the conveyance direction of the first carrier film C 1 , and then the conveyance direction is reversed by the plurality of guide rolls 19 to the same direction as that of the first carrier film C 1 .
  • the second coating portion 20 is positioned immediately above the second carrier film C 2 conveyed in the direction opposite to the conveyance direction of the first carrier film C 1 , and includes a doctor blade 21 which applies a resin composition P.
  • the resin composition P of a predetermined thickness is coated on a surface of the second carrier film C 2 by the doctor blade 21 , and a second resin sheet S 2 is formed.
  • the second resin sheet S 2 travels along with conveyance of the second carrier film C 2 .
  • the impregnation portion 22 bonds and presses the second resin sheet S 2 on the reinforcement fiber sheet F to impregnate the reinforcement fiber sheet F with the resin composition P, thereby providing a fiber-reinforced resin molding material.
  • the impregnation portion 22 is positioned on a downstream side of a position to which the reinforcement fiber sheet F on the carrier film conveying portion 14 is supplied.
  • the impregnation portion 22 includes a plurality of pressing rolls 23 .
  • the plurality of pressing rolls 23 are disposed in contact with the back surface of the second carrier film C 2 reversed in the same direction as that of the first carrier film C 1 , that is, the surface on the opposite side to the second resin sheet S 2 .
  • the first carrier film C 1 and the second carrier film C 2 are overlapped with the first resin sheet S 1 , the reinforcement fiber sheet F, and the second resin sheet S 2 sandwiched therebetween, and conveyed while being pressed by the plurality of pressing rolls 23 . Accordingly, the resin composition P of the first resin sheet S 1 and the second resin sheet S 2 is impregnated into the reinforcement fiber sheet F, and a raw sheet R 3 formed of a fiber-reinforced resin molding material is obtained.
  • the raw sheet R 3 is wound around the winder 24 .
  • the raw sheet R 3 can be cut into a predetermined length and used for molding.
  • the first carrier film C 1 and the second carrier film C 2 are peeled off from the fiber-reinforced resin molding material before molding.
  • a long first carrier film C 1 is unwound from the first raw sheet roll R 1 by the first unwinder 12 , and supplied to the carrier film conveying portion 14 .
  • a resin composition P of a predetermined thickness is coated on a surface of the first carrier film C 1 , and a first resin sheet S 1 is formed.
  • the first resin sheet S 1 on the first carrier film C 1 is caused to travel.
  • the resin composition P a resin composition having an initial viscosity of 1 Pa ⁇ s or less and having a viscosity of 5,000 Pa ⁇ s or greater and 150,000 Pa ⁇ s or less after leaving for 7 days at 25° C. after preparation is preferably used.
  • a fiber-reinforced resin molding material having a high basis weight and a low resin content can be easily manufactured.
  • the initial viscosity of the resin composition is measured at 25° C. using a B-type viscometer according to JIS 8803 immediately after the preparation of the resin composition.
  • the initial viscosity of the resin composition is preferably 0.05 Pa ⁇ s or greater and 1 Pa ⁇ s or less, more preferably 0.075 Pa ⁇ s or greater and 0.75 Pa ⁇ s or less, and even more preferably 0.1 Pa ⁇ s or greater and 0.55 Pa ⁇ s or less.
  • the initial viscosity of the resin composition is 1 Pa ⁇ s or less, more preferably 0.75 Pa ⁇ s or less, and even more preferably 0.55 Pa ⁇ s or less, the impregnation properties of the resin composition into the reinforcement fiber sheet become more excellent, and the resin composition is easily impregnated into the inside of the reinforcement fiber sheet in a thickness direction.
  • the initial viscosity of the resin composition is 0.05 Pa ⁇ s or greater, more preferably 0.075 Pa ⁇ s or greater, and even more preferably 0.1 Pa ⁇ s or greater, a high-strength fiber-reinforced resin molded article is easily obtained.
  • the viscosity of the resin composition after leaving for 7 days at 25° C. after preparation is preferably 5,000 Pa ⁇ s or greater and 150,000 Pa ⁇ s or less, more preferably 7,500 Pa ⁇ s or greater and 150,000 Pa ⁇ s or less, and even more preferably 10,000 Pa ⁇ s or greater and 150,000 Pa ⁇ s or less.
  • the viscosity of the resin composition after leaving is 5,000 Pa ⁇ s or greater, more preferably 7,500 Pa ⁇ s or greater, and even more preferably 10,000 Pa ⁇ s or greater, a high-strength fiber-reinforced resin molded article is easily obtained.
  • the impregnation properties of the resin composition into the reinforcement fiber sheet become more excellent, and the resin composition is easily impregnated into the inside of the reinforcement fiber sheet in a thickness direction.
  • the viscosity of the resin composition after leaving is measured at 25° C. using a digital viscometer HBDV-I+Prime manufactured by AMETEK, Inc. according to JIS 8803 after the prepared resin composition is left for 7 days at 25° C.
  • a reinforcement fiber sheet F is unwound from the raw sheet roll R by the reinforcement fiber sheet supply portion 10 , and continuously supplied and laminated on the first resin sheet S 1 by the guide rolls 11 .
  • a reinforcement fiber sheet formed of at least one selected from the group consisting of a unidirectional sheet in which a plurality of continuous fibers are arranged in parallel in one direction, a woven fabric in which continuous fibers are woven, and a non-crimp fabric containing continuous fibers, and having a basis weight of 200 g/m 2 or greater and 3,000 g/m 2 or less is used.
  • a long second carrier film C 2 is unwound from the second raw sheet roll R 2 by the second unwinder 18 , and a resin composition P of a predetermined thickness is coated on a surface of the second carrier film C 2 by the second coating portion 20 to form a second resin sheet S 2 .
  • the resin composition P which forms the second resin sheet S 2 the same one as the resin composition P which forms the first resin sheet S 1 is preferable.
  • the second resin sheet S 2 is caused to travel.
  • the second resin sheet S 2 is bonded on the reinforcement fiber sheet F, and pressed by the plurality of pressing rolls 23 in the impregnation portion 22 .
  • the resin composition P of the first resin sheet S 1 and the second resin sheet S 2 is impregnated into the reinforcement fiber sheet F. Accordingly, a raw sheet R 3 is obtained in which the fiber-reinforced resin molding material having the reinforcement fiber sheet F impregnated with the resin composition P is interposed between the first carrier film C 1 and the second carrier film C 2 .
  • the raw sheet R 3 is wound around the winder 24 .
  • a fiber-reinforced resin molding material with which a lightweight and high-strength fiber-reinforced resin molded article can be easily obtained can be manufactured.
  • the method for manufacturing a fiber-reinforced resin molding material according to the invention is not limited to the method using the above-described manufacturing apparatus 100 .
  • a fiber-reinforced resin molded article according to the invention is obtained by heating and pressing the fiber-reinforced resin molding material according to the invention.
  • a plurality of fiber-reinforced resin molding materials according to the invention are laminated, and then the laminate is heated under pressure applied thereto to cure the thermosetting resin.
  • the molding method is not particularly limited, and examples thereof include a press molding method, an autoclave molding method, and a bagging molding method.
  • Fiber-reinforced resin molded article according to the invention are not particularly limited, and examples thereof include sports purposes; general industrial purposes such as structural materials such as vehicles, ships, and railway vehicles; and aerospace purposes.
  • the fiber-reinforced resin molding material according to the invention is used for the fiber-reinforced resin molded article according to the invention described above, the fiber-reinforced resin molded article can be easily manufactured. In addition, it is lightweight and has a high strength.
  • an initial viscosity of a resin composition a resin composition immediately after preparation was used, and the initial viscosity was measured at 25° C. using a B-type viscometer according to JIS 8803.
  • the viscosity of the resin composition after leaving is measured at 25° C. using a digital viscometer HBDV-I+Prime manufactured by AMETEK, Inc. according to JIS 8803 after the prepared resin composition is left for 7 days at 25° C.
  • F-1 Non-crimp fabric containing continuous fibers formed of carbon fibers (product name “TKI600B”, manufactured by TK Industries, basis weight: 600 g/m 2 )
  • Non-crimp fabric containing continuous fibers formed of carbon fibers product name “TKI300UD”, manufactured by TK Industries, basis weight: 300 g/m 2 )
  • F-3 Woven fabric provided by plain weaving of continuous fibers formed of carbon fibers (product name “TR3110”, manufactured by Mitsubishi Chemical Corporation, basis weight: 200 g/m 2 )
  • F-4 Fabric containing continuous fibers formed of aramid fibers (product name “Style 1356”, manufactured by C. Cramer, Weberei, GmbH & Co. KG, basis weight: 470 g/m 2 )
  • Non-crimp fabric containing continuous fibers formed of glass fibers product name “GLASS KURAMAS UD600”, manufactured by KURABO INDUSTRIES LTD., basis weight: 625 g/m 2 )
  • P-1 Vinyl ester resin (initial viscosity: 0.3 Pa ⁇ s, viscosity after leaving: 20,000 mPa ⁇ s)
  • One fiber-reinforced resin molding material obtained in each example was used and placed on a press, and then peeled off from the press and placed again thereon. Workability (re-placing properties) during this work was evaluated according to the following evaluation criteria.
  • Tackiness (stickiness) is slightly felt, but re-placing is possible.
  • the fiber-reinforced resin molding material obtained in each example was brought into contact with a cross-section of the central portion of the reinforcement fiber sheet to evaluate impregnation properties with the following evaluation criteria.
  • the resin composition is uniformly impregnated into the reinforcement fiber sheet in a cross-section direction.
  • the resin composition is non-uniformly impregnated into the reinforcement fiber sheet in a cross-section direction.
  • a reinforcement fiber sheet F-1 was bonded to a resin surface of a resin sheet in which a polyethylene film (carrier film) was coated with a resin composition P-1 using a doctor blade such that a basis weight was 235 g/m 2 , another resin sheet was bonded to a surface on the side of the reinforcement fiber sheet F-1 in the same manner as described above, and these were pressed by a plurality of pressing rolls to obtain a fiber-reinforced resin molding material of 600 mm long ⁇ 600 mm wide.
  • the basis weight of the obtained fiber-reinforced resin molding material was 1,070 g/m 2
  • the content of the resin composition was 44 mass %
  • the fiber volume fraction was 46 volume %.
  • Fiber-reinforced resin molding materials were manufactured in the same manner as in Example 1, except that the type of the reinforcement fiber sheet to be used and the basis weight of the resin sheet were changed as shown in Table 1. Plate-like fiber-reinforced resin molded articles were manufactured in the same manner as in Example 1, except that the above fiber-reinforced resin molding materials were used.
  • a fiber-reinforced resin molding material was manufactured in the same manner as in Example 6, except that a reinforcement fiber sheet F-1 was bonded to a resin surface of a resin sheet in which a polyethylene film (carrier film) was coated with a resin composition P-1 using a doctor blade such that a basis weight was 322 g/m 2 , and a carrier film having no resin coating was laminated on a surface on the side of the reinforcement fiber sheet F-1, and a plate-like fiber-reinforced resin molded article was manufactured in the same manner as in Example 1.
  • a fiber-reinforced resin molding material was manufactured in the same manner as in Example 1, except that the basis weight of the resin sheet was changed as shown in Table 1.
  • a plate-like fiber-reinforced resin molded article was manufactured in the same manner as in Example 1, except that the above fiber-reinforced resin molding material was used.
  • Example 1 Example 2
  • Example 3 Example 4
  • Example 5 Example 6 Reinforcement Type — F-1 F-2 F-3 F-4 F-5 F-1 Fiber Sheet Basis Weight g/m 2 600 300 200 470 625 600
  • Comparative Example 1 using the fiber-reinforced resin molding material with an excessive resin composition content, the surface tackiness of the fiber-reinforced resin molding material was too high. Accordingly, it was difficult to re-laminate the fiber-reinforced resin molding materials, and the re-placing properties were poor. Furthermore, burrs were generated in the obtained fiber-reinforced resin molded article, and the moldability was inferior.
  • Comparative Example 2 using the fiber-reinforced resin molding material with an excessively small resin composition content the resin composition was non-uniformly impregnated into the reinforcement fiber sheet, and thus resin deficiency occurred and the fiber-reinforced resin molded article had poor appearance. Furthermore, since the surface tackiness was too low, the fiber-reinforced resin molding materials laminated were easily misaligned, and the lamination workability was poor.

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  • Engineering & Computer Science (AREA)
  • Mechanical Engineering (AREA)
  • Textile Engineering (AREA)
  • Chemical & Material Sciences (AREA)
  • Composite Materials (AREA)
  • Reinforced Plastic Materials (AREA)
  • Nonwoven Fabrics (AREA)
  • Woven Fabrics (AREA)
  • Moulding By Coating Moulds (AREA)
US16/655,841 2017-04-25 2019-10-17 Fiber-reinforced resin molding material and method for manufacturing same, and fiber-reinforced resin molded article Abandoned US20200047430A1 (en)

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US12269221B2 (en) 2025-04-08
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