WO2011079637A1 - Matériau composite thermoplastique renforcé par des fibres organiques à ultra-haute ténacité et résistance mécanique élevée et son procédé de préparation - Google Patents

Matériau composite thermoplastique renforcé par des fibres organiques à ultra-haute ténacité et résistance mécanique élevée et son procédé de préparation Download PDF

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Publication number
WO2011079637A1
WO2011079637A1 PCT/CN2010/077662 CN2010077662W WO2011079637A1 WO 2011079637 A1 WO2011079637 A1 WO 2011079637A1 CN 2010077662 W CN2010077662 W CN 2010077662W WO 2011079637 A1 WO2011079637 A1 WO 2011079637A1
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WO
WIPO (PCT)
Prior art keywords
fiber
nylon
thermoplastic resin
organic fiber
melting point
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PCT/CN2010/077662
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English (en)
Chinese (zh)
Inventor
杨桂生
肖玲玲
孙利明
解廷秀
Original Assignee
合肥杰事杰新材料有限公司
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Publication of WO2011079637A1 publication Critical patent/WO2011079637A1/fr

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Classifications

    • 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
    • C08J5/04—Reinforcing macromolecular compounds with loose or coherent fibrous material
    • C08J5/046—Reinforcing macromolecular compounds with loose or coherent fibrous material with synthetic macromolecular fibrous 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
    • B29K2105/00—Condition, form or state of moulded material or of the material to be shaped
    • B29K2105/0005—Condition, form or state of moulded material or of the material to be shaped containing compounding ingredients
    • B29K2105/0026—Flame proofing or flame retarding agents
    • 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
    • B29K2105/00—Condition, form or state of moulded material or of the material to be shaped
    • B29K2105/0005—Condition, form or state of moulded material or of the material to be shaped containing compounding ingredients
    • B29K2105/0044—Stabilisers, e.g. against oxydation, light or heat
    • 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
    • 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
    • B29K2105/12—Condition, form or state of moulded material or of the material to be shaped containing reinforcements, fillers or inserts of short lengths, e.g. chopped filaments, staple fibres or bristles

Definitions

  • the invention relates to an ultra high toughness high strength organic fiber reinforced thermoplastic composite material and a manufacturing method thereof
  • thermoplastic resins A commonly used method for toughening thermoplastic resins is to add an appropriate amount of a thermoplastic elastomer to the resin. For example, adding P0E, SBS, EPDM, etc. to polypropylene, adding EPDM to nylon and using a graft as a compatibilizer enhances the bond between the matrix and the elastomer.
  • the addition of elastomers can greatly increase the toughness of the thermoplastic resin, but at the same time cause a decrease in the rigidity of the material.
  • thermoplastic resins are required to increase rigidity, it is often necessary to add fillers such as inorganic particles (such as talc) or glass fibers, but the material is increased in rigidity while sacrificing the toughness of the material.
  • a single addition makes it difficult to achieve both material rigidity and toughness.
  • Organic fibers have excellent rigidity and excellent elongation and toughness. As a filler, they can improve the toughness and rigidity of materials.
  • Chinese patents CN200680017367. 8, 200680017332. 4 and Chinese patent CN200680015714. 3 disclose examples of reinforcing and toughening polypropylene with organic fibers, and mixing organic fibers and thermoplastic polypropylene through a screw extruder to obtain organic fiber reinforced and toughened poly Propylene material. Although the method mixes the organic fiber and the polypropylene well, the destruction and melting of the organic fiber due to the strong shearing of the screw makes the organic fiber as a reinforcing and toughening component not well represented.
  • the object of the invention is to obtain an ultra-high toughness and high strength organic fiber reinforced thermoplastic composite material.
  • the invention provides an ultra high toughness high strength organic fiber reinforced thermoplastic composite material, the composite material 40-90 parts by weight of thermoplastic resin,
  • the organic fiber has a melting point higher than a melting point or a processing flow temperature of the thermoplastic resin
  • the inventors have conducted extensive and intensive research to obtain an ultra-high toughness and high-strength organic fiber-reinforced thermoplastic composite material, and to improve the preparation process to achieve its ultra-high toughness while ensuring excellent tensile and bending properties.
  • the present invention has been completed on this basis.
  • the concept of the present invention is as follows:
  • the organic fiber reinforced thermoplastic composite material provided by the present invention since the organic fiber is not sheared during the melt impregnation process and controls the temperature of the melt resin, the organic fiber is not damaged in the obtained composite material.
  • the continuity of the fibers in the pellets is maintained, so that the integrity of the fibers is well maintained by subsequent injection molding and hot pressing. Therefore, the composite material has ultra-high toughness and the cantilever beam notched impact strength is as high as 5. 5JNB is constantly. At the same time, the strength and rigidity of the material are not reduced due to the greatly improved toughness, and the comprehensive properties of the material are excellent, especially showing excellent low-temperature impact.
  • ultra-high toughness and high strength means ultra-high impact strength and high tensile strength.
  • the cantilever beam notched impact strength is as high as 5. 5JNB.
  • ultrahigh molecular weight polyethylene fibers have the same meaning as in the art and are well known to those skilled in the art.
  • continuous organic fiber means an organic fiber which is not cut.
  • the ultra high toughness high strength organic fiber reinforced thermoplastic composite material comprises the following weight components:
  • the organic fiber has a melting point higher than a melting point or a processing flow temperature of the thermoplastic resin
  • the organic fiber is selected from the group consisting of nylon 6 fiber, nylon 66 fiber, nylon 46 fiber, nylon 6T fiber, nylon 9T fiber, Kevlar fiber, polyphenylene sulfide fiber, polyetheretherketone fiber, polyethylene terephthalate.
  • the organic fiber is an organic fiber having a melting point of not less than 26 CTC
  • the organic fiber having a melting point of not less than 26 CTC is selected from the group consisting of nylon 46 fiber, nylon 6T fiber, nylon 9T fiber, Kevlar fiber, and polyphenylene. Thioether fibers, or polyetheretherketone fibers.
  • the organic fibers mentioned in the present invention may be selected from the group consisting of nylon 6 fibers, nylon 66 fibers, nylon 46 fibers, nylon 6T fibers, nylon 9T fibers, Kevlar fibers, polyphenylene sulfide fibers, polyetheretherketone fibers, and poly pairs.
  • the fibers referred to in the present invention are preferably selected from the above fibers, but are not limited to the above fibers.
  • the criteria for the organic fibers selected for use in the organic fiber reinforced and toughened thermoplastic composites of the present invention are such that the melting point of the organic fibers is higher than the melting point or processing flow temperature of the thermoplastic resin to be reinforced.
  • the low melting point resin such as polyethylene, polypropylene, ABS resin, polystyrene, EVA resin or the like
  • the above-mentioned organic fibers can be used.
  • high melting point resins such as nylon 66
  • the organic fiber used has a melting point higher than the melting temperature of nylon 66 of 260 ° C, so the organic fiber used is high melting point nylon 46 fiber, nylon 6T fiber, nylon 9T fiber, Kay Fray fiber, polyphenylene sulfide fiber, polyetheretherketone fiber, and the like.
  • the inventors have found that a composite material obtained by following the above criteria can obtain ultra high toughness and high strength.
  • the thermoplastic resin may be polypropylene, polyethylene, polystyrene, ABS resin, EVA, nylon 6, nylon 66, nylon 612, nylon 1010, nylon 1212, polyethylene terephthalate, polyparaphenylene Propylene glycol formate, polybutylene terephthalate, polyphenylene ether, polyphenylene sulfide, and the like.
  • the thermoplastic resin to which the present invention relates is preferably a blend of one or more of the foregoing (for example, an ABS resin blend, more specifically, for example, a PC (polycarbonate) / ABS blend), but is not limited to the above thermoplastic Resin or blend thereof.
  • the thermoplastic resin of the present invention may be a low melting point thermoplastic resin, and the low melting point thermoplastic resin is selected from the group consisting of polyethylene, polypropylene, ABS resin, polystyrene, EVA resin, or a combination thereof.
  • the low melting point thermoplastic resin may also be modified, for example, a maleic anhydride graft modified polymer, such as maleic anhydride grafted polyethylene.
  • the thermoplastic resin may further be a thermoplastic resin having a melting point lower than the organic fiber
  • the thermoplastic resin having a melting point lower than the organic fiber is selected from the group consisting of nylon 6, nylon 66, nylon 612, nylon 1010, nylon 1212, and poly Ethylene terephthalate, polytrimethylene terephthalate, polybutylene terephthalate, polyphenylene ether, polyphenylene sulfide or a combination thereof.
  • Other ingredients are selected from the group consisting of nylon 6, nylon 66, nylon 612, nylon 1010, nylon 1212, and poly Ethylene terephthalate, polytrimethylene terephthalate, polybutylene terephthalate, polyphenylene ether, polyphenylene sulfide or a combination thereof.
  • the present invention may further contain 0 to 10 parts by weight of the compatibilizing agent, 0 to 1 part by weight of the antioxidant, and 0 to 20 parts by weight of other polymer-acceptable auxiliary agents.
  • a corresponding compatibilizer may be added.
  • some polar monomers such as: maleic anhydride or glycidyl methacrylate, acrylic acid, etc. Or a copolymer; for example, maleic anhydride grafted polypropylene, polyethylene, etc., to enhance the interfacial bonding ability between the two phases, and improve the mechanical properties of the composite.
  • antioxidants may be added to the composite to improve the overall performance of the composite.
  • other components may be added to the composite to improve the overall performance of the composite.
  • antioxidants and other polymeric acceptable auxiliaries (such as light stabilizers, lubricants, fillers, flame retardants, etc.).
  • the antioxidant is one or more of a hindered phenol, a hindered amine, a phosphite, and a thioether antioxidant, such as an antioxidant 1010, an antioxidant 168, or the like;
  • the photostabilizer is a general light stabilizer such as: 2-( 2 '-hydroxyphenyl) benzotriazole, 2-hydroxyl -4-Alkyl benzophenone, 3, 5-di-tert-butyl-4-hydroxybenzoic acid, nickel-containing light stabilizer, hindered amine light stabilizer, titanium dioxide, and the like. One or more of them are preferred according to the requirements of the materials, but are not limited to the above-listed photostabilizers.
  • the lubricant includes various waxes such as paraffin wax, polypropylene wax, polyethylene wax, amide wax and the like, and also includes small molecule compounds such as stearic acid and salts thereof and the like.
  • the lubricant of the present invention is preferably one or more of the above-mentioned lubricants, but is not limited to the above-mentioned lubricants.
  • fillers mainly refer to some or a plurality of inorganic fillers such as talc, calcium carbonate, barium sulfate, clay, kaolin, silica, wollastonite, vermiculite, and the like. But not limited to these kinds.
  • the flame retardant may be a bromine-containing flame retardant or a halogen-free flame retardant such as a phosphorus system (red phosphorus, phosphate, phosphate, etc.), a phosphorus-nitrogen system (melamine phosphate), a silicone flame retardant. Wait. Preparation
  • the material is made by the steps including the following:
  • thermoplastic resin melt (a) melting the thermoplastic resin to obtain a thermoplastic resin melt
  • the pellets are injection molded or compression molded to obtain the material;
  • the prepreg tape is subjected to hot pressing or braiding to obtain the material. More specifically, the continuous organic fiber is taken out from the creel, the tension is adjusted by the tension roller, the melt impregnation die is introduced, the fiber is dispersed and infiltrated in the die, and the fiber content is controlled by the outlet of the fiber of the die, and cooled. Curing, cutting into a fixed length (for example, 8mm, 12.5 mm, etc.) by a pelletizer, or directly into a prepreg for later hot pressing or braiding. The fibers are arranged in parallel in the pellets and the length is consistent with the length of the pellets. The length of the organic fibers in the prepreg tape is infinite, as is the length of the prepreg tape.
  • thermoplastic resin or blend and various additives are extruded into the melt-dipping mold by a single-screw extruder or a twin-screw extruder.
  • the organic fiber reinforced thermoplastic composite pellets may be processed by an injection molding process or by a hot pressing process.
  • the corresponding product can be obtained by an injection molding process.
  • the masterbatch or filler is batch mixed.
  • the masterbatch referred to in the present invention may be selected from the group consisting of flame retardant masterbatch, filled masterbatch, glass fiber long-fiber pellets, masterbatch, antistatic masterbatch, and the like.
  • the organic fiber reinforced thermoplastic composite pellets may be simultaneously mixed with one or more of the above-mentioned masterbatch according to specific performance requirements, but are not limited to the above-mentioned masterbatch, and are mainly batched according to performance requirements. Mixed.
  • the organic fiber reinforced thermoplastic composite pellets and the corresponding flame retardant masterbatch are batch-mixed and injection-molded, and composite materials with different flame retardancy levels can be obtained; in order to improve the rigidity of the composite material, the corresponding glass fiber
  • the reinforced thermoplastic composite long-fiber pellets are batch-mixed and injection-molded to improve the rigidity and heat resistance of the composite.
  • the pellets of the selected length can be directly subjected to hot pressing, or the pellets of the length of the material can be prepared or arranged to be hot pressed.
  • Other aspects of the invention will be apparent to those skilled in the art from this disclosure.
  • thermoplastic resin shown in the following Table 1 was melted according to the formulation of Table 1 below to obtain a thermoplastic resin melt; the continuous organic fibers were impregnated with the melt of the thermoplastic resin, so that the continuous organic fibers were completely wetted continuously.
  • the organic fiber is taken out from the creel, adjusted by the tension roller, enters the melt impregnation die, disperses and infiltrates the fiber in the die, controls the fiber content through the fiber outlet of the die, cools and solidifies, and is pelletized.
  • the machine is cut to a fixed length (eg 8mm, 12.5 mm, etc.).
  • the fibers are arranged in parallel in the pellets and the length is consistent with the length of the pellets.
  • the length of the organic fibers in the prepreg tape is infinite, as is the length of the prepreg tape.
  • thermoplastic resin or blend and various additives are extruded into the melt impregnation die by a single screw extruder or a twin screw extruder.
  • the pellets are injection molded or compression molded to obtain the material.
  • the corresponding product can be obtained by an injection molding process.
  • batch mixing is carried out with other masterbatches or fillers during injection molding.
  • Table 1 Injection molding process examples are mainly into distribution ratios

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  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Manufacturing & Machinery (AREA)
  • Materials Engineering (AREA)
  • Health & Medical Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Medicinal Chemistry (AREA)
  • Polymers & Plastics (AREA)
  • Organic Chemistry (AREA)
  • Reinforced Plastic Materials (AREA)
  • Compositions Of Macromolecular Compounds (AREA)

Abstract

Matériau composite thermoplastique renforcé par des fibres organiques à ultra-haute ténacité et résistance mécanique élevée, caractérisé en ce que ledit matériau composite comprend les composants suivants, en poids : résine thermoplastique, 40 à 90 parties en poids ; fibre organique, 60 à 10 parties en poids, le point de fusion de ladite fibre organique étant supérieur à celui de ladite résine thermoplastique ; compatibiliseur, 0 à 10 parties en poids ; antioxydant, 0 à 1 partie en poids ; autres additifs acceptables en science des polymères, 0 à 20 parties en poids.
PCT/CN2010/077662 2009-12-31 2010-10-12 Matériau composite thermoplastique renforcé par des fibres organiques à ultra-haute ténacité et résistance mécanique élevée et son procédé de préparation WO2011079637A1 (fr)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
CN200910247947.1 2009-12-31
CN200910247947.1A CN102115594B (zh) 2009-12-31 2009-12-31 一种超高韧性高强度有机纤维增强热塑性复合材料及其制备工艺

Publications (1)

Publication Number Publication Date
WO2011079637A1 true WO2011079637A1 (fr) 2011-07-07

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CN (1) CN102115594B (fr)
WO (1) WO2011079637A1 (fr)

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