CN103347680A - 复合成型体及其制造方法 - Google Patents

复合成型体及其制造方法 Download PDF

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Publication number
CN103347680A
CN103347680A CN2012800076550A CN201280007655A CN103347680A CN 103347680 A CN103347680 A CN 103347680A CN 2012800076550 A CN2012800076550 A CN 2012800076550A CN 201280007655 A CN201280007655 A CN 201280007655A CN 103347680 A CN103347680 A CN 103347680A
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thermoplastic resin
preform
shaped body
composite shaped
manufacture method
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CN2012800076550A
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CN103347680B (zh
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石桥壮一
越政之
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Toray Industries Inc
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Toray Industries Inc
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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
    • 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
    • B29C65/00—Joining or sealing of preformed parts, e.g. welding of plastics materials; Apparatus therefor
    • B29C65/02—Joining or sealing of preformed parts, e.g. welding of plastics materials; Apparatus therefor by heating, with or without pressure
    • 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
    • B29C65/00—Joining or sealing of preformed parts, e.g. welding of plastics materials; Apparatus therefor
    • B29C65/48—Joining or sealing of preformed parts, e.g. welding of plastics materials; Apparatus therefor using adhesives, i.e. using supplementary joining material; solvent bonding
    • B29C65/4805—Joining or sealing of preformed parts, e.g. welding of plastics materials; Apparatus therefor using adhesives, i.e. using supplementary joining material; solvent bonding characterised by the type of adhesives
    • B29C65/481—Non-reactive adhesives, e.g. physically hardening adhesives
    • B29C65/4815—Hot melt adhesives, e.g. thermoplastic adhesives
    • 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
    • B29C66/00—General aspects of processes or apparatus for joining preformed parts
    • B29C66/01—General aspects dealing with the joint area or with the area to be joined
    • B29C66/05—Particular design of joint configurations
    • B29C66/10—Particular design of joint configurations particular design of the joint cross-sections
    • B29C66/11—Joint cross-sections comprising a single joint-segment, i.e. one of the parts to be joined comprising a single joint-segment in the joint cross-section
    • B29C66/112—Single lapped joints
    • B29C66/1122—Single lap to lap joints, i.e. overlap joints
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
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    • B29C66/00—General aspects of processes or apparatus for joining preformed parts
    • B29C66/01—General aspects dealing with the joint area or with the area to be joined
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    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
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    • B29C66/00—General aspects of processes or apparatus for joining preformed parts
    • B29C66/50—General aspects of joining tubular articles; General aspects of joining long products, i.e. bars or profiled elements; General aspects of joining single elements to tubular articles, hollow articles or bars; General aspects of joining several hollow-preforms to form hollow or tubular articles
    • B29C66/51—Joining tubular articles, profiled elements or bars; Joining single elements to tubular articles, hollow articles or bars; Joining several hollow-preforms to form hollow or tubular articles
    • B29C66/54—Joining several hollow-preforms, e.g. half-shells, to form hollow articles, e.g. for making balls, containers; Joining several hollow-preforms, e.g. half-cylinders, to form tubular articles
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
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    • B29C66/72—General aspects of processes or apparatus for joining preformed parts characterised by the composition, physical properties or the structure of the material of the parts to be joined; Joining with non-plastics material characterised by the structure of the material of the parts to be joined
    • B29C66/721—Fibre-reinforced materials
    • B29C66/7212—Fibre-reinforced materials characterised by the composition of the fibres
    • 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
    • B29C66/00—General aspects of processes or apparatus for joining preformed parts
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    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
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    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
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    • B29C66/00—General aspects of processes or apparatus for joining preformed parts
    • B29C66/70—General aspects of processes or apparatus for joining preformed parts characterised by the composition, physical properties or the structure of the material of the parts to be joined; Joining with non-plastics material
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    • B29C66/723—General aspects of processes or apparatus for joining preformed parts characterised by the composition, physical properties or the structure of the material of the parts to be joined; Joining with non-plastics material characterised by the structure of the material of the parts to be joined being multi-layered
    • 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
    • B29C66/00—General aspects of processes or apparatus for joining preformed parts
    • B29C66/70—General aspects of processes or apparatus for joining preformed parts characterised by the composition, physical properties or the structure of the material of the parts to be joined; Joining with non-plastics material
    • B29C66/73—General aspects of processes or apparatus for joining preformed parts characterised by the composition, physical properties or the structure of the material of the parts to be joined; Joining with non-plastics material characterised by the intensive physical properties of the material of the parts to be joined, by the optical properties of the material of the parts to be joined, by the extensive physical properties of the parts to be joined, by the state of the material of the parts to be joined or by the material of the parts to be joined being a thermoplastic or a thermoset
    • B29C66/731—General aspects of processes or apparatus for joining preformed parts characterised by the composition, physical properties or the structure of the material of the parts to be joined; Joining with non-plastics material characterised by the intensive physical properties of the material of the parts to be joined, by the optical properties of the material of the parts to be joined, by the extensive physical properties of the parts to be joined, by the state of the material of the parts to be joined or by the material of the parts to be joined being a thermoplastic or a thermoset characterised by the intensive physical properties of the material of the parts to be joined
    • B29C66/7311—Thermal properties
    • 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
    • B29C66/00—General aspects of processes or apparatus for joining preformed parts
    • B29C66/70—General aspects of processes or apparatus for joining preformed parts characterised by the composition, physical properties or the structure of the material of the parts to be joined; Joining with non-plastics material
    • B29C66/73—General aspects of processes or apparatus for joining preformed parts characterised by the composition, physical properties or the structure of the material of the parts to be joined; Joining with non-plastics material characterised by the intensive physical properties of the material of the parts to be joined, by the optical properties of the material of the parts to be joined, by the extensive physical properties of the parts to be joined, by the state of the material of the parts to be joined or by the material of the parts to be joined being a thermoplastic or a thermoset
    • B29C66/737—General aspects of processes or apparatus for joining preformed parts characterised by the composition, physical properties or the structure of the material of the parts to be joined; Joining with non-plastics material characterised by the intensive physical properties of the material of the parts to be joined, by the optical properties of the material of the parts to be joined, by the extensive physical properties of the parts to be joined, by the state of the material of the parts to be joined or by the material of the parts to be joined being a thermoplastic or a thermoset characterised by the state of the material of the parts to be joined
    • B29C66/7377—General aspects of processes or apparatus for joining preformed parts characterised by the composition, physical properties or the structure of the material of the parts to be joined; Joining with non-plastics material characterised by the intensive physical properties of the material of the parts to be joined, by the optical properties of the material of the parts to be joined, by the extensive physical properties of the parts to be joined, by the state of the material of the parts to be joined or by the material of the parts to be joined being a thermoplastic or a thermoset characterised by the state of the material of the parts to be joined amorphous, semi-crystalline or crystalline
    • B29C66/73773—General aspects of processes or apparatus for joining preformed parts characterised by the composition, physical properties or the structure of the material of the parts to be joined; Joining with non-plastics material characterised by the intensive physical properties of the material of the parts to be joined, by the optical properties of the material of the parts to be joined, by the extensive physical properties of the parts to be joined, by the state of the material of the parts to be joined or by the material of the parts to be joined being a thermoplastic or a thermoset characterised by the state of the material of the parts to be joined amorphous, semi-crystalline or crystalline the to-be-joined area of at least one of the parts to be joined being semi-crystalline
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    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
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    • B29C66/00—General aspects of processes or apparatus for joining preformed parts
    • B29C66/70—General aspects of processes or apparatus for joining preformed parts characterised by the composition, physical properties or the structure of the material of the parts to be joined; Joining with non-plastics material
    • B29C66/73—General aspects of processes or apparatus for joining preformed parts characterised by the composition, physical properties or the structure of the material of the parts to be joined; Joining with non-plastics material characterised by the intensive physical properties of the material of the parts to be joined, by the optical properties of the material of the parts to be joined, by the extensive physical properties of the parts to be joined, by the state of the material of the parts to be joined or by the material of the parts to be joined being a thermoplastic or a thermoset
    • B29C66/737—General aspects of processes or apparatus for joining preformed parts characterised by the composition, physical properties or the structure of the material of the parts to be joined; Joining with non-plastics material characterised by the intensive physical properties of the material of the parts to be joined, by the optical properties of the material of the parts to be joined, by the extensive physical properties of the parts to be joined, by the state of the material of the parts to be joined or by the material of the parts to be joined being a thermoplastic or a thermoset characterised by the state of the material of the parts to be joined
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    • B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
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    • 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
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    • B29C65/10—Joining or sealing of preformed parts, e.g. welding of plastics materials; Apparatus therefor by heating, with or without pressure using hot gases (e.g. combustion gases) or flames coming in contact with at least one of the parts to be joined
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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
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    • B29C65/02—Joining or sealing of preformed parts, e.g. welding of plastics materials; Apparatus therefor by heating, with or without pressure
    • B29C65/14—Joining or sealing of preformed parts, e.g. welding of plastics materials; Apparatus therefor by heating, with or without pressure using wave energy, i.e. electromagnetic radiation, or particle radiation
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
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    • B29C65/14—Joining or sealing of preformed parts, e.g. welding of plastics materials; Apparatus therefor by heating, with or without pressure using wave energy, i.e. electromagnetic radiation, or particle radiation
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    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
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    • B29C65/20—Joining or sealing of preformed parts, e.g. welding of plastics materials; Apparatus therefor by heating, with or without pressure using heated tools with direct contact, e.g. using "mirror"
    • 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
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    • B29C65/02—Joining or sealing of preformed parts, e.g. welding of plastics materials; Apparatus therefor by heating, with or without pressure
    • B29C65/18—Joining or sealing of preformed parts, e.g. welding of plastics materials; Apparatus therefor by heating, with or without pressure using heated tools
    • B29C65/22—Heated wire resistive ribbon, resistive band or resistive strip
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
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    • B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
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    • B29C65/34—Joining or sealing of preformed parts, e.g. welding of plastics materials; Apparatus therefor by heating, with or without pressure using heated elements which remain in the joint, e.g. "verlorenes Schweisselement"
    • B29C65/3404—Joining or sealing of preformed parts, e.g. welding of plastics materials; Apparatus therefor by heating, with or without pressure using heated elements which remain in the joint, e.g. "verlorenes Schweisselement" characterised by the type of heated elements which remain in the joint
    • B29C65/3436—Joining or sealing of preformed parts, e.g. welding of plastics materials; Apparatus therefor by heating, with or without pressure using heated elements which remain in the joint, e.g. "verlorenes Schweisselement" characterised by the type of heated elements which remain in the joint comprising independent continuous fibre-reinforcements
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    • B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
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    • B29C65/34—Joining or sealing of preformed parts, e.g. welding of plastics materials; Apparatus therefor by heating, with or without pressure using heated elements which remain in the joint, e.g. "verlorenes Schweisselement"
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    • B29C65/34—Joining or sealing of preformed parts, e.g. welding of plastics materials; Apparatus therefor by heating, with or without pressure using heated elements which remain in the joint, e.g. "verlorenes Schweisselement"
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    • B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
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    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
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  • Engineering & Computer Science (AREA)
  • Mechanical Engineering (AREA)
  • Chemical & Material Sciences (AREA)
  • Physics & Mathematics (AREA)
  • Crystallography & Structural Chemistry (AREA)
  • Mathematical Physics (AREA)
  • Composite Materials (AREA)
  • Thermal Sciences (AREA)
  • Laminated Bodies (AREA)
  • Reinforced Plastic Materials (AREA)
  • Lining Or Joining Of Plastics Or The Like (AREA)

Abstract

本发明提供一种复合成型体的制造方法以及通过该方法制造的复合成型体，所述复合成型体的制造方法中，(1)由纤维增强热塑性树脂构成的预成型体a、b的至少一方含有重均纤维长1mm以上的增强纤维，(2)预成型体a使用热塑性树脂A，预成型体b使用热塑性树脂A或者热塑性树脂B，(3)在预成型体a、b的任一者、或者预成型体a、b二者的表面上形成热塑性树脂C的薄膜，(4)在将树脂C配置于接合的界面处的状态下，通过加热使热塑性树脂C、以及预成型体a、b的一部分熔融，通过该熔融将预成型体a、b接合，制造复合成型体。通过使热塑性树脂C的结晶化速度相对地变慢，能够使树脂C以更长时间与预成型体a、b的表面以熔融状态相接，从而实现预成型体a、b之间的高强度接合。

Description

复合成型体及其制造方法
技术领域
本发明涉及复合成型体及其制造方法，特别是涉及对预先成型为规定形状的由使用热塑性树脂的纤维增强树脂构成的预成型体进行加热使预成型体的一部分熔融、在该熔融部位进行预成型体之间的接合、从而成型为复合成型体的、复合成型体的制造方法以及通过该方法制造的复合成型体。
背景技术
已知将热固性树脂的纤维增强树脂与热塑性树脂的纤维增强树脂进行接合、制造作为整体由纤维增强树脂构成的复合成型体的方法(例如专利文献1、2)。热塑性树脂自身以及使用热塑性树脂的纤维增强树脂，能够比较容易地进行注射成型等，因此，与热固性树脂以及使用其的纤维增强树脂相比，成型性和批量生产率优良。因此，特别是在大批量生产的商品等的制造中，要求能够将使用热塑性树脂的纤维增强树脂之间高效地接合的复合成型体的制造方法。
作为这样的复合成型体的制造方法，例如，可以考虑如下方法。即，准备至少2种使用已经通过加压成型或注射成型赋形的热塑性树脂的纤维增强树脂制品(例如使用聚苯硫醚(PPS)的纤维增强树脂制品、将其称为预成型体或者一次成型品)，通过直接加热、振动、超声波等任意方法进行加热，同时将预成型体之间进行压接，由此，使预成型体的一部分熔融，通过由该熔融引起的接合，形成复合成型体。通过这样的所谓的熔合，能够得到例如作为配置有中空结构体、肋部等的兼具强度和刚性的最终成型品的复合成型体。
但是，例如，使用如上所述的通常的PPS级的预成型体中，PPS树脂的结晶化速度比较快，因此，作为结果，从熔融状态开始冷却时的固化快。其结果，即使给予一定热量使预成型体的表面熔解，也会在进行压接等实现良好熔合的步骤之前发生快速固化，因此，不能得到期待程度的接合强度。因此，有可能作为最终成型品的复合成型体的强度和刚性不能达到目标值。
专利文献1：日本专利第3906319号公报
专利文献2：日本专利第4543696号公报
发明内容
因此，本发明的课题在于提供一种能够高效地制造复合成型体的方法、以及通过该方法制造的复合成型体，所述方法在制造使用成型性和批量生产率优良的热塑性树脂的纤维增强树脂的复合成型体时，使已经预先成型的预成型体之间以充分高的接合强度熔合，能够高效地制造作为强度和刚性优良的最终成型品的复合成型体。
为了解决上述课题，本发明的复合成型体的制造方法，将使用纤维增强热塑性树脂预先成型的预成型体a与使用纤维增强热塑性树脂预先成型的预成型体b接合、成型为复合成型体，其特征在于，
(1)预成型体a及b的至少一方含有重均纤维长为1mm以上的增强纤维，
(2)预成型体a使用热塑性树脂A，预成型体b使用热塑性树脂A或者热塑性树脂B，
(3)在预成型体a或者b的任一者、或者预成型体a及b二者的表面上形成热塑性树脂C的薄膜，
(4)在将热塑性树脂C的薄膜配置于接合的界面处的状态下，通过加热使热塑性树脂C以及预成型体a以及b的一部分熔融，通过由该熔融引起的接合，成型为复合成型体。
作为包含上述重均纤维长为1mm以上的增强纤维的预成型体，例如可以采用下述(1)成形体及(2)成型体中的任一者或者采用由它们组合形成的成型体：
(1)成型体，由毡片状基材与热塑性树脂的组合形成，所述毡片状基材是重均纤维长为1mm～50mm的范围的增强纤维实质上随机取向而成的，
(2)成型体，以在预成型体的任意的二个端部之间的范围内配置连续纤维的方式被增强。
即，在使用热塑性树脂的纤维增强树脂的成型品中，例如，为了实现显示出作为结构材料所要求的高力学特性，需要增强纤维长度较长，因此，优选重均纤维长1mm以上的增强纤维，特别是考虑到成型性等，优选为使用重均纤维长为1mm～50mm的范围的增强纤维的增强纤维基材的成型品，优选通过将该范围的纤维长的增强纤维实质上随机取向而成的毡片状基材与热塑性树脂组合而成的成型体。或者，也优选以在预成型体的任意的二个端部之间(例如，成为对向的2边的两端部之间)的范围内配置增强纤维(形成为连续纤维)的方式被增强的成型体。进而，也可以采用它们组合而成的形式的成型体。
如上所述，作为预成型体，使用以在任意的二个端部之间的范围内配置连续纤维的方式被增强的成型体是本发明的优选方式之一。在这样的方式中，不产生纤维的断裂，在使用某些增强纤维的情况下能够得到最高力学特性。如果将该连续纤维增强的预成型体以结构的骨架材料的方式配置，则本发明的复合一体成型品能够同时实现高力学特性和复杂的形状。
作为预成型体的增强纤维，在使用不连续增强纤维的情况下，优选由其重均纤维长如上所述为1mm～50mm的增强纤维构成。重均纤维长低于1mm时，不会产生增强纤维的特性，无法发挥所要求的高力学特性。重均纤维长超过50mm时，损害在形成不连续增强纤维时的一个特征即良好的赋形性。
另外，特别重视耐冲击性等力学特性的情况下，可以将包含上述重均纤维长1mm以上的增强纤维的预成型体中的、增强纤维的重均纤维长为20mm～50mm的范围作为更优选的范围示出。这是由于，如后述的图2所示，关于对以耐冲击性为代表的力学特性提高的贡献，纤维长度影响很大。
该不连续纤维的取向等没有特别限定，可以使用实质上随机取向的不连续纤维。作为该实质上随机的范围，可以例示在面内各向同性分散的、或者具有平缓的一定取向的片状的毡片，其可以使用通过造纸法、梳理法、气流法等已知的纤维毡片制造法制成的毡片。
另外，作为本发明的优选方式之一，也可以列举如下方式：包含上述重均纤维长1mm以上的增强纤维的预成型体的至少表层部由如下部分形成，所述部分包含将由连续纤维构成的增强纤维单向取向而成的层。
上述热塑性树脂A、热塑性树脂B以及热塑性树脂C，可以使用彼此不同的配方的热塑性树脂(即，为同种的热塑性树脂，但为了使物性或特性彼此不同而通过彼此不同的配方制备的热塑性树脂)。由于为热塑性树脂之间的接合方式，所以本质上易于得到容易良好接合的状态，另外，也容易将成型品整体粉碎进行再利用(再循环)。本发明中，即使为热塑性树脂之间的接合，预成型体也预先成型，因此，为了使形成预成型体的表层部的热塑性树脂C、与热塑性树脂A或者热塑性树脂B之间具有高接合强度，特别是为了实现该目标，本发明中可以采用如下方式。例如上述热塑性树脂A、热塑性树脂B以及热塑性树脂C以结晶性的热塑性树脂作为主成分、并且满足以下关系。
热塑性树脂C的结晶化温度＜热塑性树脂A的结晶化温度、以及
热塑性树脂C的结晶化温度＜热塑性树脂B的结晶化温度
这样，通过采用对结晶化温度赋予高低的差的方式，特别使位于接合的界面处的热塑性树脂C的结晶化温度相对地降低，结晶化速度能够减缓(结晶化温度越高结晶化速度越快)，在通过施加振动等加热接合面时，能够在结晶化前使界面的热塑性树脂C充分地熔融，能够获得对预成型体之间进行压接等使界面相容的时间。由此，能够制造在使用热塑性树脂A、热塑性树脂B的预成型体之间的组合中以高接合强度进行接合的复合成型体。需要说明的是，关于该结晶化温度(Tc)的测定，通过差示扫描量热计(DSC)将对象树脂从熔融状态开始以一定速度(10℃/分钟)进行冷却，测定结晶化发热峰温度[结晶化温度(Tc)]，由此，评价上述结晶化速度(结晶化温度(Tc)越高结晶化速度越快)。
另外，为了满足如上所述的结晶化温度特性，或者，上述结晶化温度特性之外的性质，可以采用如下方式：上述热塑性树脂A以及热塑性树脂B是由将特定的单体进行聚合而成的均聚物构成的热塑性树脂，并且上述热塑性树脂C是由下述共聚物构成的热塑性树脂、或者混合该共聚物而成的树脂组成物，所述共聚物是通过2种以上不同的单体共聚而得到的共聚物，该2种以上的单体之一包含与热塑性树脂A或者热塑性树脂B相同的单体。在这样的方式中，能够使热塑性树脂C侧的结晶化温度与热塑性树脂A或热塑性树脂B侧相比降低，该结晶化速度慢的热塑性树脂C经过较长的时间与热塑性树脂A以及热塑性树脂B以熔融状态相接，从而能够实现与热塑性树脂A或热塑性树脂B的(预成型体a与预成型体b之间的)高强度接合。即，能够制造以高接合强度进行接合的复合成型体。
需要说明的是，降低热塑性树脂A、热塑性树脂B以及热塑性树脂C全部树脂的结晶化温度，能够使体系整体的结晶化速度变慢。但是，如果对整体体系采用降低结晶化速度的特别的方法，则无法避免成本上升，该方法不能认为是工业上有利的方法。通过仅仅在接合的界面使用结晶化温度相对较低的热塑性树脂C，能够得到两者的充分的接合强度，并且能够避免成本大幅上升。
作为上述接合部的边界层(中间层)，可以采用使用热塑性树脂C的、例如膜、或者通过熔喷或纺粘等形成的无纺布。其配置在预成型体a或者预成型体b的任一者或者预成型体a及预成型体b二者的表面上。例如，通过加压等预先得到预成型体时，优选预先配置在表面上，预先进行一体化。该情况下，即使热塑性树脂C与热塑性树脂A或者热塑性树脂B部分地混合，热塑性树脂C在表面上部分地露出也没有关系。
作为本发明的复合成型体的制造方法中的、预成型体a与预成型体b的接合方法，例如，可以使用如下方法。可以列举：振动熔敷(利用在2种预成型体的接合界面处产生的摩擦热，使树脂熔融进行熔敷的方法)、热板熔合(对要熔敷的预成型体用已经预先加热的热板通过接触或者非接触方式进行加热，接合面达到熔融状态后，对2种预成型体加压进行熔敷的技术)、脉冲熔合(以低电压、大电流对加热线进行短时间通电，使其发热，作为热源的熔合方法)、高频熔合(利用高频的感应加热作用，使接合物(导电体)引起内部发热进行熔敷的工艺)、超声波熔合(利用通过对预成型体赋予纵向的超声波振动而产生的摩擦热，局部瞬间地升温的方法)等。此外，也可以使用：通过电磁感应加热使导电体(例如碳纤维)中通过感应电流，通过焦耳热使其发热的方法；在导电体(例如碳纤维)中直接通电，通过焦耳热使其发热的方法；利用热风、焊矩、激光器的方法等已知的加热方法。
作为本发明的复合成型体的制造方法中的、更具体的热塑性树脂A及热塑性树脂B与热塑性树脂C的组合，例如可以举出如下组合。例如可以列举：热塑性树脂A及热塑性树脂B以对聚苯硫醚作为主成分、热塑性树脂C由共聚聚苯硫醚构成的组合。该情况下，作为共聚聚苯硫醚，可以使用对苯硫醚单元与间苯硫醚单元共聚而成的聚合物。
使用聚苯硫醚的方式为本发明的最优选的方式之一。聚苯硫醚是具有刚直的骨架的聚合物，具有高刚性，通过与碳纤维等增强纤维组合，显示出高力学特性。因此，即使增强纤维的重均纤维长较短，为1mm～20mm，也显示出比较高的力学特性。进而，在纤维长更长、为连续增强纤维的情况下，显示出更高的特性。另外为难燃性，优选用于各种电子设备或汽车用电装部件等要求难燃性的用途。另外，对于通常的以对聚苯硫醚作为主体的聚苯硫醚，结晶化速度快，通常是难以进行复合一体成型的体系，但通过采用本发明，例如，热塑性树脂C使用降低结晶化温度的(使结晶化速度变慢的)树脂体系，由此，能够得到接合强度高的复合成型体。
另外，作为其他组合，也可以采用热塑性树脂A及热塑性树脂B由聚酰胺构成、热塑性树脂C由共聚聚酰胺构成的方式。
需要说明的是，本发明的热塑性树脂A及热塑性树脂B与热塑性树脂C的组合不限于上述例子。优选热塑性树脂C的结晶化温度比热塑性树脂A或热塑性树脂B低，用于实现其的方法也没有限定。作为使高分子的结晶化温度变化的方法，可以利用公知的技术，除了使用上述共聚物的方法以外，还可以通过滑石、高岭土、有机磷化合物、特定聚合物的少量添加等、添加各种结晶核剂来控制结晶化温度。另外，通过使热塑性树脂A、热塑性树脂B、热塑性树脂C的主聚合物链的末端为特定的基团，也能够使结晶化温度变化。
另外，在本发明的复合成型体的制造方法中，作为所使用的增强纤维的种类，没有特别限定，可以使用碳纤维、玻璃纤维、芳族聚酰胺纤维等，也可以为将这些组合的混合构成。在以复合成型体的制造的强度设计或制造的容易性等为目的的情况下，特别优选包含碳纤维的方式。特别是在使用了连续纤维的预成型体的增强纤维中使用碳纤维时，能够使其较高的增强纤维特征最强地发挥。
本发明中，也提供通过如上所述的方法制造的复合成型体。制造的复合成型体的形状和结构没有特别限定。预成型体a与预成型体b的熔合部，优选确保为其形状允许的范围内的宽面积。也能够形成嵌合形状。预成型体的至少一方，可以例示使用通常的注射成型机注射颗粒样的材料而得到的预成型体。另外，也可以使用进行与其类似的动作的成型方法。例如，也可以使用将注射与加压的动作组合的所谓的注射加压成型。用于注射成型及其类似技术的颗粒，可以是通常的复合颗粒，也可以是所谓的长纤维颗粒。
这样，根据本发明的复合成型体的制造方法，将预成型体a与预成型体b进行接合时，使形成预成型体的表层部的热塑性树脂C、与另外使用的热塑性树脂A或者热塑性树脂B为同种但彼此不同配方的热塑性树脂，使热塑性树脂C的结晶化速度相对地较慢，因此，该热塑性树脂C经过更长时间与热塑性树脂A以及热塑性树脂B以熔融状态进行相接，从而能够实现树脂A或树脂B的(预成型体a与预成型体b之间的)高强度接合。如上所述制造的复合成型体具有高机械强度和刚性，另外是同种的热塑性树脂之间的接合体，因此，可以形成还兼具优良的再循环性能的复合成型体。
附图说明
图1是表示本发明的一个实施方式的复合成型体的制造方法的构成简图。
图2是针对本发明表示增强纤维的纤维长与复合特性及成型性的一般关系的特性图。
具体实施方式
以下，参照附图对本发明的实施方式进行说明。
图1中示出了本发明的一个实施方式的复合成型体的制造方法和本发明中的预成型体的结构例。图1中，1表示预成型体a，2表示预成型体b。另外，3表示使用结晶化温度相对较低的热塑性树脂C(例如低结晶化温度PPS[低结晶化温度共聚聚苯硫醚])的层。在预成型体a(1)的单面上预先一体地形成由热塑性树脂C形成的层3。预成型体a(1)以及预成型体b(2)分别由使用了结晶化温度与热塑性树脂C相比相对较高的热塑性树脂A、热塑性树脂B(例如通常的结晶化温度的PPS)的纤维增强树脂构成。
如上所述的预成型体a(1)以及预成型体b(2)，一边通过直接加热、振动、超声波等适当的方法进行加热一边将预成型体之间进行压接，由此，使预成型体的一部分熔融、通过由该熔融引起的接合，制作复合成型体4。通过如上所述的所谓的熔合，例如，得到作为配置有中空结构体、和肋部的兼具有强度·刚性的最终成型品的复合成型体4。
一般认为也存在预成型体b(2)中使用的树脂为与热塑性树脂A不同的热塑性树脂B的情况。另外，热塑性树脂C的层3可以预先形成在预成型体a(1)的表层上，也可以预先形成在预成型体b(2)的表层上，只要是在熔合面上存在热塑性树脂C的方式，则可以使用任意一种情况。也可以在预成型体a(1)及预成型体b(2)的两者的表层上形成热塑性树脂C的层3。
上述预成型体a、b通过加压成型或注射成型等成型法得到，对其成型方法没有特别限定。使用加压成型的情况下，例如，在织布等连续纤维基材、单向地排列纤维而成的基材(单向性基材[UD])、长纤维毡片等中复合或浸渗热塑性树脂，将如上所述形成的所谓的热塑性预浸料坯作为原材料，将其置于模具内，进行加热、加压，成型规定的形状的预成型体即可。此时，例如，在模具的最下层或者最上层预先配置由热塑性树脂C形成的膜或无纺布等，然后进行加压，由此能够实现一体化。另外，在注射成型的情况下，也可以如下成型：在模具的腔室内也预先配置由热塑性树脂C形成的膜或无纺布等，或预先在腔室内配置热塑性预浸料坯，然后，通过进行注射成型的嵌件成型等方法来成型。此外，可以采用所谓的注射加压成型、真空成型、吹塑成型、高压釜成型、膜片成型等已知的热塑性树脂成型技术用于得到预成型体。预成型体通常在1次成型后为了脱模而进行冷却，之后，再次被加热/接合，加工成复合成型体。例如也可以举出：虽然通过不同的成型机使预成型体a与预成型体b分别成型、但通过接下来的工序自动接合的联合生产线等。当然预成型体a与预成型体b的成型循环如果不同，也可以采用独立的接合加工生产线。
能够以良好的接合强度使预成型体之间自由地接合、复合，由此作为其最终形态的复合成型体的形状以及设计自由度显著地提高。例如，通过通常的注射成型难以得到的中空结构等也可以容易地实现。另外，例如，使用具有高力学特性的连续纤维增强预浸料坯来成型具有缓和曲面的面板部(预成型体a)，在其上接合具有用于加强的肋部等的复杂形状注射成型品(预成型体b)，由此能够同时实现复杂的形状和高力学特性。此时如果适当地以形成中空部的方式进行接合，则能够进一步使轻质性也大幅提高。预成型体a、b和各自使用的原材料、形状可以在其能够使用的原材料的适用范围内自由地设定。采用重均纤维长20mm以上的长纤维或连续纤维增强，并且以PPS树脂这样的高弹性模量、高耐热性树脂作为基体树脂的基质，使预成型体a为面板形状(例如表层面板)，使预成型体b为L通道、C通道、I通道、Ω通道等形态(例如纵梁)，将这些预成型体之间接合从而构成整体表层面板(integral skin panel)结构，为上述结构时也可以适用于飞机用结构材料这样的要求高力学特性和轻量性的结构。同样地在面板形状(例如外板)上接合加强构件(例如内框)的汽车结构用途也可以容易地实现。需要说明的是，此时，相对于宽面板形状的预成型体a而言，接合多个作为增强材料的预成型体b的构成，也包括在本发明内。
为了考察纤维增强树脂的组合对接合强度的影响度，采用如图1所示的预成型体的组合进行振动熔合试验。预成型体a以及预成型体b中，作为热塑性树脂A、B均使用通常结晶化温度的聚苯硫醚，在预成型体a的单侧表面上一体地形成热塑性树脂C的层。作为热塑性树脂C，使用结晶化温度低的聚苯硫醚树脂。该情况下，接合强度高，接合强度的偏差小。为了与其进行比较，准备除了不含热塑性树脂C之外其他所有条件均相同的预成型体a以及预成型体b，进行熔合试验，结果，接合强度低，接合强度的偏差大。
上述中，关于以PPS作为基质的热塑性树脂A、热塑性树脂B以及热塑性树脂C的组合进行了例示。例如如上所述，该组合可以列举：热塑性树脂A以及热塑性树脂B由聚苯硫醚构成、热塑性树脂C由共聚聚苯硫醚构成的组合，作为共聚聚苯硫醚，可以使用例如对苯硫醚单元与间苯硫醚单元共聚而成的聚合物。本发明中，除了这样的以PPS作为基质的热塑性树脂A、热塑性树脂B、热塑性树脂C的组合以外，例如，如上所述，也可以采用热塑性树脂A以及热塑性树脂B由聚酰胺构成、热塑性树脂C由共聚聚酰胺构成的组合方式。使用这样的共聚聚酰胺的情况下，作为能够共聚的聚酰胺形成性成分的例子，可以列举：6-氨基己酸(不包括a-1的情况)、11-氨基十一酸、12-氨基十二烷酸、对氨基甲基苯甲酸等氨基酸、ε-氨基己内酰胺(不包括a-1的情况)、ω-十二内酰胺等内酰胺、丁二胺、己二胺、2-甲基戊二胺、十一烷二胺、十二烷二胺、2，2，4-/2，4，4-三甲基己二胺、5-甲基壬二胺、间苯二甲胺、对苯二甲胺、1，3-双(氨基甲基)环己烷、1，4-双(氨基甲基)环己烷、1-氨基-3-氨基甲基-3，5，5-三甲基环己烷、双(4-氨基环己基)甲烷、双(3-甲基-4-氨基环己基)甲烷、2，2-双(4-氨基环己基)丙烷、双(氨基丙基)哌嗪、氨基乙基哌嗪等脂肪族、脂环族、芳香族的二胺、以及己二酸、辛二酸、壬二酸、癸二酸、十二烷二酸、对苯二甲酸、间苯二甲酸、2-氯对苯二甲酸、2-甲基对苯二甲酸、5-甲基间苯二甲酸、间苯二甲酸-5-磺酸钠、六氢对苯二甲酸、六氢间苯二甲酸等脂肪族、脂环族、芳香族的二羧酸。另外，根据想要得到的成型品的要求特性，可以在树脂中添加难燃剂、耐候性改良剂、以及抗氧化剂、热稳定剂、紫外线吸收剂、增塑剂、润滑剂、着色剂、相溶化剂、导电性填料等。
另外，本发明中，预成型体使用包含重均纤维长1mm以上的增强纤维的第1纤维增强树脂进行预先成型，优选例如为下述(1)成形体及(2)成型体中的任一者或者是它们组合形成的成型体，
(1)成型体，由毡片状基材与树脂的组合形成，所述毡片状基材是重均纤维长为1mm～50mm的范围的增强纤维实质上随机取向而成的，
(2)成型体，以在该预成型体的任意的二个端部之间的范围内配置连续纤维的方式被增强。
如上规定的原因在于，对于预成型体自身及作为最终成型品的复合成型体的、各种机械特性和成型性·赋型性来说，通过如上规定使双方均满足良好的特性。
即，图2中给出了纤维增强树脂(复合)中的、成型材料中包含的增强纤维的长度(重均纤维长、单位：mm)与经成型的纤维增强树脂的各种特性的相对水平之间的一般关系，如其所示，纤维长缩短时，弹性模量、强度、耐冲击性降低，但成型性·赋型性良好，相反，纤维长增长时，弹性模量、强度、耐冲击性增高，但成型性·赋型性变差。为了均衡性良好地且保持这些特性较高，特别优选含有重均纤维长为1mm～50mm的范围的增强纤维。
图2中，同时例示了与成型材料中包含的增强纤维的长度(重均纤维长)对应的代表的成型工艺(注射成型、加压成型、高压釜成型、RTM成型[Resin Transfer Molding])(当然并不限于这些成型工艺)，在为本发明的优选方案的情况下、即含有重均纤维长为1mm～50mm的范围的增强纤维的情况下，适合加压成型。
产业上的可利用性
本发明的复合成型体及其制造方法，可适用于所有复合成型体的用途中，特别是在高效地以优良的生产率制造要求比较大量生产的复合成型体的情况下优选使用。作为本发明的复合成型体的用途，例如可以举出：个人电脑、显示器、OA设备、手机、便携信息终端、传真机、只读光盘、便携式MD、便携式收放音机、PDA(电子笔记本等便携信息终端)、数码相机、数码静态相机、光学设备、音响、空调、照明设备、娱乐用品、玩具用品、其他家电制品等电气、电子设备的壳体以及盘、底盘等内部构件或其容器、机构部件、面板等建材用途、马达部件、交流发电机端子、交流发电机连接器、IC调节器、调光器用电位计、悬挂部件、排气阀等各种阀门、燃料相关、排气系统或者吸气系统各种管道、进气喷嘴通气管、吸入歧管、各种机械臂、各种框、各种转轴、各种轴承、燃料泵、汽油罐、CNG罐、发动机冷却水套管、汽化器主体、汽化器衬垫、排气传感器、冷却水传感器、油温传感器、制动磨擦片磨损传感器、节气门位置传感器、曲轴、位置传感器、空气流量计、制动磨擦片磨耗传感器、空调用恒温器基质、供暖热风流量控制阀门、散热器起动机用电刷架、水泵叶轮、涡轮机叶片、雨刮电机有关零件、分配器、起动机开关、起动继电器、变速器用束线、窗清洗器喷嘴、空调面板开关基板、燃料关系电磁气阀用线圈、保险丝用连接器、电池托盘、AT托架、前照灯支架、踏板护罩、方向盘、门梁、保护装置、底盘、框、扶手、霍恩终端、步进电动机转子、灯座、灯反光镜、灯罩、制动活塞、噪声屏蔽、散热器支架、备用轮胎罩、座壳、电磁线、发动机机油滤清器、点火装置箱、底盖、踏板、支柱装饰部件、传动轴、车轮、挡泥板、盘座面、保险杠、保险杠横梁、发动机罩、气体配件、平台、前罩板通风孔、车顶、仪表板、阻流板以及各种模块等的汽车、二轮车相关零件、构件以及外板或起落架舱、翼片、阻流板、边缘、指针、升降机、整流罩、肋等飞机相关零件、构件以及外板等。
符号说明
1预成型体a
2预成型体b
3热塑性树脂C的层
4复合成型体

Claims (11)

1.一种复合成型体的制造方法，所述制造方法将使用纤维增强热塑性树脂预先成型的预成型体a与使用纤维增强热塑性树脂预先成型的预成型体b接合、成型复合成型体，其特征在于，
(1)预成型体a及b的至少一方含有重均纤维长为1mm以上的增强纤维，
(2)预成型体a使用热塑性树脂A，预成型体b使用热塑性树脂A或者热塑性树脂B，
(3)在预成型体a或者b的任一者、或者预成型体a及b二者的表面上形成热塑性树脂C的薄膜，
(4)在将热塑性树脂C的薄膜配置于接合的界面处的状态下，通过加热使热塑性树脂C以及预成型体a及b的一部分熔融，通过由所述熔融引起的接合，成型复合成型体。
2.如权利要求1所述的复合成型体的制造方法，其中，所述含有重均纤维长为1mm以上的增强纤维的预成型体为下述(1)成型体及(2)成型体中的任一者或者是它们组合形成的成型体，
(1)成型体，由毡片状基材与热塑性树脂的组合形成，所述毡片状基材是重均纤维长为1mm～50mm的范围的增强纤维实质上随机取向而成的，
(2)成型体，以在预成型体的任意的二个端部之间的范围内配置连续纤维的方式被增强。
3.如权利要求2所述的复合成型体的制造方法，其中，所述含有重均纤维长为1mm以上的增强纤维的预成型体是由毡片状基材与热塑性树脂的组合形成的成型体，所述毡片状基材是重均纤维长为20mm～50mm的范围的增强纤维实质上随机取向而成的。
4.如权利要求1所述的复合成型体的制造方法，其中，所述含有重均纤维长为1mm以上的增强纤维的预成型体的至少表层部由如下部分形成，所述部分包含将由连续纤维形成的增强纤维单向取向而成的层。
5.如权利要求1～4中任一项所述的复合成型体的制造方法，其中，所述热塑性树脂A、热塑性树脂B及热塑性树脂C以结晶性的热塑性树脂作为主成分，并且满足以下关系，
热塑性树脂C的结晶化温度＜热塑性树脂A的结晶化温度、及
热塑性树脂C的结晶化温度＜热塑性树脂B的结晶化温度。
6.如权利要求1～5中任一项所述的复合成型体的制造方法，其中，所述热塑性树脂A及热塑性树脂B是由将特定的单体进行聚合而成的均聚物形成的热塑性树脂，并且所述热塑性树脂C是由下述共聚物形成的热塑性树脂、或者是混合所述共聚物而成的树脂组合物，所述共聚物是由2种以上的不同的单体共聚形成的共聚物，所述2种以上的单体的之一中含有与热塑性树脂A或者热塑性树脂B中的单体相同的单体。
7.如权利要求1～6中任一项所述的复合成型体的制造方法，其中，所述热塑性树脂A及热塑性树脂B以聚苯硫醚作为主成分，所述热塑性树脂C由共聚聚苯硫醚形成。
8.如权利要求7所述的复合成型体的制造方法，其中，所述共聚聚苯硫醚由对苯硫醚单元与间苯硫醚单元进行共聚而成的聚合物形成。
9.如权利要求1～6中任一项所述的复合成型体的制造方法，其中，所述热塑性树脂A及热塑性树脂B以聚酰胺作为主成分，所述热塑性树脂C由共聚聚酰胺形成。
10.如权利要求1～9中任一项所述的复合成型体的制造方法，其中，所述预成型体a及b的至少一者含有碳纤维作为增强纤维。
11.一种复合成型体，其通过权利要求1～10中任一项所述的方法制造。
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