WO2019220914A1 - 複合材の製造方法および複合材 - Google Patents

複合材の製造方法および複合材 Download PDF

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Publication number
WO2019220914A1
WO2019220914A1 PCT/JP2019/017623 JP2019017623W WO2019220914A1 WO 2019220914 A1 WO2019220914 A1 WO 2019220914A1 JP 2019017623 W JP2019017623 W JP 2019017623W WO 2019220914 A1 WO2019220914 A1 WO 2019220914A1
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Prior art keywords
resin
composite material
prepreg
layer
laminated
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Ceased
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PCT/JP2019/017623
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English (en)
French (fr)
Japanese (ja)
Inventor
幸生 武内
秋山　勝徳
駿一 森島
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Mitsubishi Heavy Industries Ltd
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Mitsubishi Heavy Industries Ltd
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Application filed by Mitsubishi Heavy Industries Ltd filed Critical Mitsubishi Heavy Industries Ltd
Priority to US16/629,810 priority Critical patent/US11370183B2/en
Priority to CN201980003682.2A priority patent/CN110997268A/zh
Priority to EP19803166.8A priority patent/EP3647012A4/en
Publication of WO2019220914A1 publication Critical patent/WO2019220914A1/ja
Anticipated expiration legal-status Critical
Ceased 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
    • B29C70/28—Shaping operations therefor
    • B29C70/40—Shaping or impregnating by compression not applied
    • B29C70/42—Shaping or impregnating by compression not applied for producing articles of definite length, i.e. discrete articles
    • B29C70/44—Shaping or impregnating by compression not applied for producing articles of definite length, i.e. discrete articles using isostatic pressure, e.g. pressure difference-moulding, vacuum bag-moulding, autoclave-moulding or expanding rubber-moulding
    • B29C70/443—Shaping or impregnating by compression not applied for producing articles of definite length, i.e. discrete articles using isostatic pressure, e.g. pressure difference-moulding, vacuum bag-moulding, autoclave-moulding or expanding rubber-moulding and impregnating by vacuum or injection
    • 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
    • B29C43/00—Compression moulding, i.e. applying external pressure to flow the moulding material; Apparatus therefor
    • B29C43/02—Compression moulding, i.e. applying external pressure to flow the moulding material; Apparatus therefor of articles of definite length, i.e. discrete articles
    • B29C43/10—Isostatic pressing, i.e. using non-rigid pressure-exerting members against rigid parts or dies
    • B29C43/12—Isostatic pressing, i.e. using non-rigid pressure-exerting members against rigid parts or dies using bags surrounding the moulding material or using membranes contacting the moulding material
    • 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
    • B29C43/00—Compression moulding, i.e. applying external pressure to flow the moulding material; Apparatus therefor
    • B29C43/32—Component parts, details or accessories; Auxiliary operations
    • B29C43/34—Feeding the material to the mould or the compression means
    • 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
    • B29C43/00—Compression moulding, i.e. applying external pressure to flow the moulding material; Apparatus therefor
    • B29C43/32—Component parts, details or accessories; Auxiliary operations
    • B29C43/56—Compression moulding under special conditions, e.g. vacuum
    • 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
    • B29C70/08—Fibrous reinforcements only comprising combinations of different forms of fibrous reinforcements incorporated in matrix material, forming one or more layers, and with or without non-reinforced layers
    • B29C70/081—Combinations of fibres of continuous or substantial length and short fibres
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
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    • 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
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    • B29C70/10—Fibrous reinforcements only characterised by the structure of fibrous reinforcements, e.g. hollow fibres
    • B29C70/12—Fibrous reinforcements only characterised by the structure of fibrous reinforcements, e.g. hollow fibres using fibres of short length, e.g. in the form of a mat
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    • 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
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    • B29C70/10—Fibrous reinforcements only characterised by the structure of fibrous reinforcements, e.g. hollow fibres
    • B29C70/12—Fibrous reinforcements only characterised by the structure of fibrous reinforcements, e.g. hollow fibres using fibres of short length, e.g. in the form of a mat
    • B29C70/14—Fibrous reinforcements only characterised by the structure of fibrous reinforcements, e.g. hollow fibres using fibres of short length, e.g. in the form of a mat oriented
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    • 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
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    • 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
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
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    • 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
    • B29C70/28—Shaping operations therefor
    • B29C70/40—Shaping or impregnating by compression not applied
    • B29C70/42—Shaping or impregnating by compression not applied for producing articles of definite length, i.e. discrete articles
    • B29C70/44—Shaping or impregnating by compression not applied for producing articles of definite length, i.e. discrete articles using isostatic pressure, e.g. pressure difference-moulding, vacuum bag-moulding, autoclave-moulding or expanding rubber-moulding
    • 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
    • B29C70/28—Shaping operations therefor
    • B29C70/54—Component parts, details or accessories; Auxiliary operations, e.g. feeding or storage of prepregs or SMC after impregnation or during ageing
    • B29C70/542—Placing or positioning the reinforcement in a covering or packaging element before or during moulding, e.g. drawing in a sleeve
    • 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
    • B29C70/28—Shaping operations therefor
    • B29C70/54—Component parts, details or accessories; Auxiliary operations, e.g. feeding or storage of prepregs or SMC after impregnation or during ageing
    • B29C70/543—Fixing the position or configuration of fibrous reinforcements before or during moulding
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B37/00—Methods or apparatus for laminating, e.g. by curing or by ultrasonic bonding
    • B32B37/0007—Methods or apparatus for laminating, e.g. by curing or by ultrasonic bonding involving treatment or provisions in order to avoid deformation or air inclusion, e.g. to improve surface quality
    • B32B37/003—Methods or apparatus for laminating, e.g. by curing or by ultrasonic bonding involving treatment or provisions in order to avoid deformation or air inclusion, e.g. to improve surface quality to avoid air inclusion
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B37/00—Methods or apparatus for laminating, e.g. by curing or by ultrasonic bonding
    • B32B37/14—Methods or apparatus for laminating, e.g. by curing or by ultrasonic bonding characterised by the properties of the layers
    • B32B37/16—Methods or apparatus for laminating, e.g. by curing or by ultrasonic bonding characterised by the properties of the layers with all layers existing as coherent layers before laminating
    • B32B37/18—Methods or apparatus for laminating, e.g. by curing or by ultrasonic bonding characterised by the properties of the layers with all layers existing as coherent layers before laminating involving the assembly of discrete sheets or panels only
    • B32B37/182—Methods or apparatus for laminating, e.g. by curing or by ultrasonic bonding characterised by the properties of the layers with all layers existing as coherent layers before laminating involving the assembly of discrete sheets or panels only one or more of the layers being plastic
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
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    • B32B5/00—Layered products characterised by the non- homogeneity or physical structure, i.e. comprising a fibrous, filamentary, particulate or foam layer; Layered products characterised by having a layer differing constitutionally or physically in different parts
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    • B32B5/22—Layered products characterised by the non- homogeneity or physical structure, i.e. comprising a fibrous, filamentary, particulate or foam layer; Layered products characterised by having a layer differing constitutionally or physically in different parts characterised by the presence of two or more layers which are next to each other and are fibrous, filamentary, formed of particles or foamed
    • B32B5/24—Layered products characterised by the non- homogeneity or physical structure, i.e. comprising a fibrous, filamentary, particulate or foam layer; Layered products characterised by having a layer differing constitutionally or physically in different parts characterised by the presence of two or more layers which are next to each other and are fibrous, filamentary, formed of particles or foamed one layer being a fibrous or filamentary layer
    • B32B5/26—Layered products characterised by the non- homogeneity or physical structure, i.e. comprising a fibrous, filamentary, particulate or foam layer; Layered products characterised by having a layer differing constitutionally or physically in different parts characterised by the presence of two or more layers which are next to each other and are fibrous, filamentary, formed of particles or foamed one layer being a fibrous or filamentary layer another layer next to it also being fibrous or filamentary
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08J—WORKING-UP; GENERAL PROCESSES OF COMPOUNDING; AFTER-TREATMENT NOT COVERED BY SUBCLASSES C08B, C08C, C08F, C08G or C08H
    • C08J5/00—Manufacture of articles or shaped materials containing macromolecular substances
    • C08J5/24—Impregnating materials with prepolymers which can be polymerised in situ, e.g. manufacture of prepregs
    • 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
    • B29K2101/00—Use of unspecified macromolecular compounds as moulding material
    • B29K2101/10—Thermosetting resins
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    • B29K2105/00—Condition, form or state of moulded material or of the material to be shaped
    • B29K2105/06—Condition, form or state of moulded material or of the material to be shaped containing reinforcements, fillers or inserts
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Definitions

  • This disclosure relates to a method for manufacturing a composite material and a composite material.
  • FRP Fiber Reinforced Plastics
  • Patent Document 1 a composite material is manufactured by the former method using a laminate formed by laminating a plurality of reinforcing fabrics formed by reinforcing fiber yarns.
  • the “prepreg” used in the latter is a sheet-like intermediate material in which a reinforcing fiber is impregnated with an uncured resin and the curing reaction of the resin is stopped halfway to facilitate handling.
  • a method of laminating the prepreg in an arbitrary direction and pressure-curing and molding with an autoclave is the most reliable and high-quality means.
  • the composite material includes laminated fiber reinforced layers (reinforced fabric or prepreg).
  • the molded product in which the fiber reinforced layer is laminated has low toughness between the fiber reinforced layer and the fiber reinforced layer (interlayer). For this reason, the molded product often breaks due to cracks between the layers.
  • the crack propagation direction is often the in-plane direction S of the fiber reinforced layer.
  • Examples of methods for increasing the toughness between layers include the following (1) to (3).
  • FIG. 3 is a schematic cross-sectional view in the thickness direction of a composite material 20 in which elastomer particles (rubber particles) 21 are dispersed in a matrix resin.
  • the composite material 20 in which a soft material such as the elastomer particles 21 is dispersed the elastomer particles 21 bounce when a load is applied, and there is room for deformation of the resin due to the generated voids. Thereby, the composite material 20 of FIG. 3 can absorb fracture energy by shearing deformation.
  • the elastomer particles 21 are dispersed, the particle size and dispersion state of the elastomer particles 21 are required to be controlled, and a toughness improving agent adding step is required later.
  • the elastomer particles 21 are added to the matrix resin, the amount of the matrix resin is relatively reduced, so that the strength of the composite material is reduced.
  • FIG. 4 is a schematic cross-sectional view in the thickness direction of a composite material 30 in which a thermoplastic resin 32 is introduced between the fiber reinforced layer 31 and the fiber reinforced layer 31.
  • the inserted thermoplastic resin 32 has a large elongation and a thermally stable property.
  • the interlayer thermoplastic resin 32 contributes to the toughness improvement of the composite material.
  • the thermoplastic resin 32 has a higher effect of improving toughness than the elastomer particles 21 of FIG.
  • the thermoplastic resin 32 when the thermoplastic resin 32 is introduced, it is necessary to manage the particle size and dispersion state of the thermoplastic resin 32, resulting in high costs. Furthermore, there are problems such as severe restrictions on the rate of temperature rise due to the thermally stable state of the thermoplastic resin 32 and the matrix resin.
  • FIG. 5 is a schematic cross-sectional view in the thickness direction of a composite 40 of a three-dimensional woven fabric in which reinforcing fibers are oriented in the thickness direction T. Since the reinforcing fibers are oriented in the thickness direction, the toughness reinforcing effect between the layers is high. On the other hand, the three-dimensional woven fabric is more expensive to manufacture than the conventional woven fabric, and the fiber orientation in the in-plane direction S is reduced, so that the strength as the composite material 40 is reduced. In the three-dimensional woven fabric, the fibers oriented in the thickness direction are arranged to avoid the fiber bundles oriented in the in-plane direction S.
  • the meandering and misalignment of the fiber bundle that occurs at this time can be a factor for reducing the strength of the composite material 40. Furthermore, in a three-dimensional woven fabric, it is common to impregnate a resin after preparing a fiber reinforced layer in a desired shape, and it is difficult to adopt a method using a prepreg.
  • the present disclosure has been made in view of such circumstances, and an object thereof is to provide a method of manufacturing a composite material that improves interlayer strength.
  • An object of the present disclosure is to provide a cheaper composite material having improved interlayer strength.
  • the manufacturing method and the composite material of the present disclosure employ the following means.
  • the present disclosure relates to a method for manufacturing a composite material in which a plurality of prepregs impregnated with an uncured matrix resin are laminated on a fiber reinforced base material, and is heat-molded. And a resin layer disposed on both sides of the gap layer, a plurality of short fibers are disposed on the opposing surfaces of the adjacent prepregs and the prepreg, and the laminated prepreg is evacuated to Provided is a method for producing a composite material that is heat-molded after degassing a void layer.
  • the present disclosure is directed to a laminate in which a plurality of fiber reinforced substrates are laminated, a cured matrix resin filled in the laminate, and a direction different from an in-plane direction of the fiber reinforced substrate, and adjacent And a plurality of short fibers existing between the fiber-reinforced substrates.
  • the short fibers arranged between the prepreg and the prepreg are in contact with the matrix resin.
  • the short fiber is changed in orientation as the matrix resin heated and flowable flows into the void layer, and is oriented in a direction different from the in-plane direction of the fiber reinforced base material.
  • a short fiber comes to span between adjacent fiber reinforced base materials.
  • Short fibers existing between adjacent fiber reinforced substrates reinforce the bonding between adjacent fiber reinforced substrates (interlayers). According to the said invention, the interlayer reinforcement effect comparable as a three-dimensional fabric can be acquired.
  • a prepreg provided with a resin layer on both sides of a void layer has a better positioning of the prepreg during lamination than a prepreg provided with a resin layer only on one side.
  • the plurality of prepregs are preferably stacked with the same side facing in the same direction. Thereby, the toughness between a plurality of layers can be made comparable.
  • the resin layers disposed on both sides of the gap layer have different thicknesses
  • the matrix resin included in the resin layer is preferably a thermosetting resin or a thermosetting resin and a curing agent thereof.
  • “consisting of” permits “including only additives” and “not including thermoplastic resin, elastomer and toughness improver, but including other additives”.
  • “Toughness improvers” include rubbers such as nitrile rubber, thermoplastic resins that are compatible with matrix resins (for example, polyethersulfone when the matrix resin is an epoxy resin), and long lengths between the crosslinking points. Examples thereof include a chain matrix resin or a resin highly compatible with the matrix resin, a benzoxazine resin having a hydrogen bond in a layered form and an increased shear deformability.
  • “Other additives” include ultraviolet absorbers, flame retardants, thickening and viscosity modifiers, internal mold release agents, lubricants, and the like.
  • thermosetting resins that do not contain thermoplastic resins, elastomers, and toughness improvers are less expensive than thermosetting resins that contain them.
  • a thermosetting resin that does not contain a toughness improver has a high crosslink density, so that the curing temperature is close to the glass transition temperature.
  • Thermosetting resins that do not contain thermoplastic resins, elastomers, and toughness improvers have a simple curing reaction because they do not contain any additional additives, so when producing prepregs with a void layer and composite materials It is easy to manage the temperature etc. Thereby, the matrix resin and the reinforcing fiber can be selected on the user side according to the application.
  • the short fibers have a length equal to or greater than the thickness of the gap layer. Therefore, even when the matrix resin moves by the thickness of the void layer, it can exist between adjacent fiber-reinforced substrates if the short fibers are oriented in the thickness direction of the prepreg.
  • the method for manufacturing a composite material according to the present disclosure can be applied to an aircraft structural part made of carbon fiber reinforced plastic (CFRP).
  • CFRP carbon fiber reinforced plastic
  • the method for manufacturing a composite material according to the present disclosure is preferably applied to a primary structural member of an aircraft that requires a residual strength after application of an impact.
  • the composite manufacturing method according to the present disclosure has a low impact resistance requirement compared to the primary structural member, but the secondary structural member (fairing) of an aircraft that is easily manufactured at low cost and further weight reduction is required. , Nacelle cover, etc.).
  • the composite material manufacturing method according to the present disclosure can be applied to parts that require impact properties in general industrial machines (for example, forklifts, platform doors installed at railway station platforms).
  • a method for manufacturing a composite material according to the present embodiment will be described with reference to FIG.
  • a composite material is manufactured by laminating a plurality of prepregs 10 impregnated with an uncured matrix resin on a fiber reinforced base material and then heat-molding it.
  • stacking two prepregs is illustrated in FIG. 1, the number of lamination
  • prepreg lamination For the prepreg 10, a semi-impregnated prepreg having a void layer 12 between the resin layers (11a, 11b) is used. The semi-impregnated prepreg will be described in detail later.
  • a plurality of short fibers 13 are disposed on the opposing surfaces of the adjacent prepreg 10 and prepreg 10. After the lamination, the plurality of short fibers 13 are in contact with the matrix resin of the prepreg 10.
  • the short fibers are, for example, nanocellulose fibers and have a thickness of 10 to 100 microns.
  • Short fibers for example, some acrylic fibers, nylon fibers, from the unit area weight per 10 g / m 2 in the short fiber mat material, such as glass fibers 100 g / m 2.
  • the next prepreg 10 is laminated on one prepreg 10 so as to sandwich the short fibers 13.
  • the arrangement of the short fibers 13 and the lamination of the prepregs 10 may be repeated a predetermined number of times in accordance with the above.
  • the prepreg 10 has a front side surface with a resin layer 11a and a back side surface with a resin layer 11b.
  • the plurality of prepregs 10 are all preferably laminated with the same side facing the same direction.
  • the thicknesses of the resin layers (11a, 11b) arranged on both surfaces of the gap layer 12 are different (when the gap layer 12 is biased toward one of the prepregs 10 in the thickness direction T of the prepreg). It is desirable to laminate a plurality of prepregs 10 with the thin resin layer 11b facing upward in the lamination direction.
  • the thinner resin layers 11b are laminated to face each other. “Different thickness” refers to a case where there is a difference of 100 ⁇ m or more when the resin thickness is compared.
  • the “thickness direction T” of the prepreg is a direction that intersects at a substantially right angle to the surface of the prepreg, and substantially corresponds to the same direction as the lamination direction of the prepreg.
  • Deaeration is performed at a vacuum degree of 200 mmHg or less, preferably 150 mmHg or less. In order to prevent the degassed gas from returning to the laminate, it is preferable that the vacuum is always drawn during the molding. “Sufficient” is 10 minutes or more.
  • the void layer 12 itself acts as a deaeration circuit. Insufficient deaeration is not preferable because it may block the deaeration circuit.
  • Heating is started after the void layer 12 is sufficiently degassed.
  • an oven or a heater mat is used in addition to the autoclave.
  • the heating is performed in at least three stages: first heating for raising the temperature from normal temperature to a predetermined temperature, second heating for raising the temperature from the predetermined temperature to the molding temperature, and third heating for maintaining the molding temperature for a predetermined time and curing the matrix resin. To do.
  • the temperature increase rate in the first heating is preferably 10 ° C./min or less.
  • the temperature increase rate in the second heating is preferably 10 ° C./min or less.
  • the predetermined temperature is 100 ° C. or higher.
  • the molding temperature is a temperature at which the matrix resin can be cured. Since the prepreg used in this embodiment does not contain additives such as a thermoplastic resin and an elastomer, the molding temperature and the predetermined time may simply conform to the characteristics of the matrix resin. The molding temperature and the predetermined time may be conditions recommended by the manufacturer of the matrix resin to be used.
  • the viscosity of the matrix resin decreases once and becomes flowable.
  • the matrix resin having a lowered viscosity flows into the void layer 12 and fills the voids of the fiber reinforced substrate.
  • the short fibers 13 that are in contact with the matrix resin are drawn into the neighboring fiber reinforced substrate as the matrix resin flows. Since the matrix resin flows in the thickness direction, the short fibers 13 are also oriented in a direction different from the in-plane direction S of the prepreg 10 ′ (mainly the thickness direction T of the prepreg 10 ′).
  • the prepreg 10 may be pressurized (for example, at 2 to 3 atmospheres) at the timing when the viscosity of the matrix resin decreases.
  • pressurizing the heating temperature is adjusted so that the temperature increase rate of the second heating does not exceed the desired range.
  • pressure By applying pressure, the flow of the matrix resin into the void layer 12 can be promoted.
  • a laminate in which a plurality of fiber reinforced substrates are laminated, a cured matrix resin filled in the laminate, and a direction different from the in-plane direction of the fiber reinforced substrate. And a composite material comprising a plurality of short fibers 13 existing between a plurality of fiber-reinforced substrates.
  • the short fiber 13 oriented in a direction different from the in-plane direction S of the fiber reinforced base material may exist between a plurality of fiber reinforced base materials.
  • joining (interlayer) between a fiber reinforced base material and a fiber reinforced base material is strengthened, and as a result, toughness is improved.
  • Fiber reinforced base material examples include a unidirectional material in which fiber bundles are aligned in one direction (longitudinal direction), a nonwoven fabric, and a woven fabric.
  • the fibers used for the fiber reinforced substrate are carbon fibers, glass fibers, organic fibers, inorganic fibers other than glass, and the like.
  • the thickness of the fiber reinforced substrate is preferably 0.05 mm or more and 0.5 mm or less.
  • thermosetting resin As the matrix resin, a heat-resistant thermosetting resin is used.
  • the high heat-resistant thermosetting resin can be selected from resin materials that are widely used for molds or jigs. Specifically, the thermosetting resin is an epoxy resin, a polyester resin, a vinyl ester resin, a cyanate ester resin, a polyimide resin, or the like. “High heat resistance” can be defined depending on the application of the composite. For example, an aircraft structural member means that it can withstand heat of 150 ° C. or higher.
  • the matrix resin may include a thermosetting resin and its curing agent.
  • the matrix resin does not include a thermoplastic resin, an elastomer, a long chain resin, or the like.
  • the matrix resin may contain additives such as an internal mold release agent, a flame retardant, an ultraviolet absorber, and a lubricant.
  • the addition rate of the additive is less than 20% by weight of the total amount of the matrix resin, preferably less than 10% by weight, more preferably 0% by weight.
  • thermosetting resin that does not contain a thermoplastic resin and an elastomer is less expensive than a toughness improving type resin mixed with an elastomer and a thermoplastic resin.
  • the prepreg is an intermediate material obtained by impregnating a fiber reinforced base material with an uncured matrix resin.
  • FIG. 2 illustrates a cross-sectional view in the thickness direction of the prepreg used in the present embodiment.
  • the prepreg 10 used in the present embodiment is a semi-impregnated prepreg.
  • the semi-impregnated prepreg includes a void layer 12 and resin layers (11a, 11b) disposed on both sides of the void layer 12.
  • the void layer 12 is a layer composed of a fiber reinforced base material (not shown) that does not contain a matrix resin.
  • the gap layer 12 is continuous in the in-plane direction S.
  • the thickness of the gap layer 12 is preferably 0.1 mm to half the thickness of one layer.
  • the thickness of the gap layer 12 in FIG. 2 is 0.1 mm.
  • Resin layers (11a, 11b) cover both surfaces of the fiber reinforced substrate (void layer 12).
  • the resin layers (11a, 11b) are layers composed of a fiber reinforced base material and a matrix resin impregnated therein.
  • the thickness of the resin layer 11a in FIG. 2 is equal to or greater than the gap layer thickness.
  • Semi-impregnated prepregs are prepared by applying a pre-made matrix resin film to both sides of a fiber reinforced substrate, applying vacuum and applying heat to impregnate the matrix resin into the fiber reinforced substrate. It can be produced by stopping the reaction near the gel point of the matrix resin before impregnating the whole material.
  • the void layer 12 may be formed biased toward the vertical lower surface side of the fiber reinforced base material. This is a bias that occurs as a result of the resin impregnation on one side becoming deeper because the fiber position is fixed when the fibers are aligned in one direction and only one side is impregnated quickly with resin during prepreg manufacture.
  • the curing reaction can be made to simply depend on the properties of the thermosetting resin. As a result, the curing reaction can be easily managed, so that the void layer 12 having a desired thickness can be formed.
  • the short fibers 13 may be fibers that are soft and easy to be drawn into the flow of the matrix resin.
  • the short fibers 13 are polyamide fibers (for example, nylon), cellulose fibers, glass fibers, polyester fibers, and the like.
  • the short fiber 13 is longer than the thickness of the void layer. Specifically, the length of the short fiber 13 is 0.1 mm or more.
  • the short fiber 13 If the short fiber 13 is too thick, it is difficult to be drawn into the fiber reinforced base material. When the short fiber 13 is too thin, the handleability is lowered. When the short fiber 13 is too thin, the reinforcing effect is lowered. The prepreg surface is somewhat sticky at room temperature. Therefore, if the short fiber 13 satisfies the above-mentioned diameter range, it can be held on the prepreg surface by the stickiness only by being sprinkled on the prepreg surface.
  • Prepreg (with void layer) 10 'prepreg (gap layer impregnated with matrix resin) 11a, 11b Resin layer 12 Void layer 13 Short fiber 20, 30, 40 Composite 21 Elastomer particle 31 Fiber reinforced layer 32 Thermoplastic resin

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PCT/JP2019/017623 2018-05-18 2019-04-25 複合材の製造方法および複合材 Ceased WO2019220914A1 (ja)

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KR102472506B1 (ko) * 2021-07-02 2022-12-01 한국항공우주산업 주식회사 복합재 제조 방법
EP4509306A4 (en) * 2022-12-07 2025-08-13 Resonac Corp METAL-CLAD LAMINATE, PRINTED CIRCUIT BOARD, SEMICONDUCTOR PACKAGE AND MANUFACTURING METHOD THEREOF
WO2024122587A1 (ja) * 2022-12-07 2024-06-13 株式会社レゾナック プリプレグ、積層板、金属張り積層板、プリント配線板、半導体パッケージ並びにプリプレグの製造方法及び金属張り積層板の製造方法
CN116512636A (zh) * 2023-05-25 2023-08-01 东风商用车有限公司 一种复合材料板簧及其成型方法
CN119840198A (zh) * 2023-10-17 2025-04-18 上海飞机制造有限公司 一种复合材料像质计及其制备方法与应用

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US20210008818A1 (en) 2021-01-14
CN110997268A (zh) 2020-04-10
EP3647012A4 (en) 2020-11-18

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