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CN102405255A - 熔接用聚对苯二甲酸丁二醇酯树脂组合物及复合成形品 - Google Patents

熔接用聚对苯二甲酸丁二醇酯树脂组合物及复合成形品 Download PDF

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Publication number
CN102405255A
CN102405255A CN2010800165057A CN201080016505A CN102405255A CN 102405255 A CN102405255 A CN 102405255A CN 2010800165057 A CN2010800165057 A CN 2010800165057A CN 201080016505 A CN201080016505 A CN 201080016505A CN 102405255 A CN102405255 A CN 102405255A
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CN
China
Prior art keywords
polybutylene terephthalate
terephthalate resin
welding
resin composition
molded article
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Granted
Application number
CN2010800165057A
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CN102405255B (zh
Inventor
坂田耕一
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POLY PLASTICS CO Ltd
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Wintech Polymer Ltd
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    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08K—Use of inorganic or non-macromolecular organic substances as compounding ingredients
    • C08K5/00—Use of organic ingredients
    • C08K5/16—Nitrogen-containing compounds
    • C08K5/29—Compounds containing one or more carbon-to-nitrogen double bonds
    • 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
    • B29C65/06—Joining or sealing of preformed parts, e.g. welding of plastics materials; Apparatus therefor by heating, with or without pressure using friction, e.g. spin welding
    • 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
    • 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
    • B29C65/16—Laser beams
    • B29C65/1629—Laser beams characterised by the way of heating the interface
    • B29C65/1635—Laser beams characterised by the way of heating the interface at least passing through one of the parts to be joined, i.e. laser transmission welding
    • 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
    • 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
    • B29C65/16—Laser beams
    • B29C65/1629—Laser beams characterised by the way of heating the interface
    • B29C65/1654—Laser beams characterised by the way of heating the interface scanning at least one of the parts to be joined
    • 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
    • B29C66/12—Joint cross-sections combining only two joint-segments; Tongue and groove joints; Tenon and mortise joints; Stepped joint cross-sections
    • B29C66/122—Joint cross-sections combining only two joint-segments, i.e. one of the parts to be joined comprising only two joint-segments in the joint cross-section
    • B29C66/1222—Joint cross-sections combining only two joint-segments, i.e. one of the parts to be joined comprising only two joint-segments in the joint cross-section comprising at least a lapped joint-segment
    • 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
    • B29C66/05—Particular design of joint configurations
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    • B29C66/122—Joint cross-sections combining only two joint-segments, i.e. one of the parts to be joined comprising only two joint-segments in the joint cross-section
    • B29C66/1224—Joint cross-sections combining only two joint-segments, i.e. one of the parts to be joined comprising only two joint-segments in the joint cross-section comprising at least a butt joint-segment
    • 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
    • B29C66/05—Particular design of joint configurations
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    • B29C66/124—Tongue and groove joints
    • B29C66/1244—Tongue and groove joints characterised by the male part, i.e. the part comprising the tongue
    • B29C66/12443—Tongue and groove joints characterised by the male part, i.e. the part comprising the tongue having the tongue substantially in the middle
    • 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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    • B29C66/13—Single flanged joints; Fin-type joints; Single hem joints; Edge joints; Interpenetrating fingered joints; Other specific particular designs of joint cross-sections not provided for in groups B29C66/11 - B29C66/12
    • B29C66/131—Single flanged joints, i.e. one of the parts to be joined being rigid and flanged in the joint area
    • 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
    • B29C66/20—Particular design of joint configurations particular design of the joint lines, e.g. of the weld lines
    • B29C66/24—Particular design of joint configurations particular design of the joint lines, e.g. of the weld lines said joint lines being closed or non-straight
    • B29C66/242—Particular design of joint configurations particular design of the joint lines, e.g. of the weld lines said joint lines being closed or non-straight said joint lines being closed, i.e. forming closed contours
    • B29C66/2422—Particular design of joint configurations particular design of the joint lines, e.g. of the weld lines said joint lines being closed or non-straight said joint lines being closed, i.e. forming closed contours being circular, oval or elliptical
    • B29C66/24221—Particular design of joint configurations particular design of the joint lines, e.g. of the weld lines said joint lines being closed or non-straight said joint lines being closed, i.e. forming closed contours being circular, oval or elliptical being circular
    • 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
    • B29C66/50—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
    • B29C66/53—Joining single elements to tubular articles, hollow articles or bars
    • B29C66/534—Joining single elements to open ends of tubular or hollow articles or to the ends of bars
    • B29C66/5346—Joining single elements to open ends of tubular or hollow articles or to the ends of bars said single elements being substantially flat
    • B29C66/53461—Joining single elements to open ends of tubular or hollow articles or to the ends of bars said single elements being substantially flat joining substantially flat covers and/or substantially flat bottoms to open ends of container bodies
    • 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
    • B29C66/50—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
    • B29C66/542—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 joining hollow covers or hollow bottoms to open ends of container bodies
    • 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
    • B29C66/50—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
    • B29C66/61—Joining from or joining on the inside
    • 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
    • B29C66/50—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
    • B29C66/65—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 with a relative motion between the article and the welding tool
    • B29C66/652—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 with a relative motion between the article and the welding tool moving the welding tool around the fixed article
    • 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
    • B29C66/71—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 composition of the plastics material of the parts to be joined
    • 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
    • B29C66/739—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 material of the parts to be joined being a thermoplastic or a thermoset
    • B29C66/7392—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 material of the parts to be joined being a thermoplastic or a thermoset characterised by the material of at least one of the parts being a thermoplastic
    • B29C66/73921—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 material of the parts to be joined being a thermoplastic or a thermoset characterised by the material of at least one of the parts being a thermoplastic characterised by the materials of both parts being thermoplastics
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08K—Use of inorganic or non-macromolecular organic substances as compounding ingredients
    • C08K5/00—Use of organic ingredients
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    • C08K5/11—Esters; Ether-esters of acyclic polycarboxylic acids
    • 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
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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
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    • B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
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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
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    • B29C66/7315—Mechanical properties
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Abstract

本发明的目的在于提供一种在通过热熔接加工方法而一体化时保持高熔接强度并且在冷热循环环境下的耐久性优异的聚对苯二甲酸丁二醇酯树脂材料。详细而言，所述熔接用聚对苯二甲酸丁二醇酯树脂组合物中，相对于100重量份(A)末端羧基量为30meq/kg以下的聚对苯二甲酸丁二醇酯树脂，配混以下成分而成：(B)碳二亚胺化合物：设(A)聚对苯二甲酸丁二醇酯树脂的末端羧基量为1时，碳二亚胺官能团量为0.3～1.5当量的量；(C)弹性体：0～15重量份。

Description

熔接用聚对苯二甲酸丁二醇酯树脂组合物及复合成形品
技术领域
本发明涉及熔接用聚对苯二甲酸丁二醇酯树脂组合物及复合成形品。
背景技术
以聚对苯二甲酸丁二醇酯(PBT)为代表的热塑性聚酯树脂具有优异的耐热性、耐化学药品性、电特性、机械特性、成形流动性等，被广泛用于汽车电装部件(各种控制单元、点火线圈部件)、发动机部件、各种传感器部件、连接器部件、开关部件、继电器部件、线圈部件、变压器部件、灯部件等汽车领域、电气·电子领域中。在这些部件中，聚酯树脂主要作为电子部件保护用的外装材料使用，所以，会形成多种部件，作为其接合方法，一直以来采用螺纹紧固或粘接、热熔接等。
但是，在螺纹紧固中，嵌入螺母、螺栓、垫圈等所花费的费用、连接的费事、重量增加成为问题。此外，粘接剂很多情况下到固化为止有时间的损失、需要固定夹具，存在伴随于此的成本增加的问题，此外从环境保护的方面出发溶剂的使用成为问题。
另一方面，以激光熔接、振动熔接、超声波熔接、热板熔接、旋转熔接等为代表的热熔接由于能够在短时间内接合，不使用粘接剂、螺栓等金属部件，所以不会产生其耗费成本、重量增加、环境污染等问题，利用该方法的组装逐渐增加。
此外，作为电子部件保护用的外装材料使用时，大多埋入用于传递电信号的金属端子等，但对于设置在汽车发动机室等温度升降剧烈的环境中的部件而言，由于金属与树脂的线性膨胀差所产生的变形而容易产生裂纹，损害部件的功能，所以，为了防止裂纹，大多使聚对苯二甲酸丁二醇酯中含有弹性体等来改良韧性，并提出了各种组合物。
例如，日本特开平3-285945号公报中公开了通过在聚对苯二甲酸丁二醇酯中添加丙烯酸亚乙基烷基酯等弹性体来提高耐热冲击性的方法。但是，与无添加的产品相比虽然可确认到改善效果，但有时耐热冲击性仍不充分。
此外，日本特开昭60-210659号公报中公开了通过在聚对苯二甲酸丁二醇酯中添加丙烯酸亚乙基烷基酯等弹性体和环氧树脂或碳二亚胺来提高耐热水性的方法。但是，该组合物虽然提高了耐热水性，但耐热冲击性不充分。
进而，日本特开2004-315805号公报中公开了通过使用聚对苯二甲酸丁二醇酯和特定折射率的弹性体来改善激光熔接性和热冲击性的方法。但是，该组合物中，为了提高热冲击性而增加弹性体量时，在振动熔接等中由于弹性体的聚集，存在成为熔接不良的原因、熔接强度其自身降低之类的问题。
如上所述，一直以来众所周知的是为了改良韧性而配混弹性体，但对于为了改良韧性而配混必要量的弹性体时熔接强度降低之类的问题尚无解决方法。
发明内容
本发明是鉴于上述现有技术的问题而研究出的，本发明的目的在于，提供一种在将由聚对苯二甲酸丁二醇酯树脂形成的成形品通过以激光熔接、振动熔接、超声波熔接、热板熔接、旋转熔接等为代表的热熔接加工方法一体化时保持高熔接强度并且在冷热循环环境下的耐久性优异的聚对苯二甲酸丁二醇酯树脂材料。
本发明人等为了获得可达成上述目的的聚对苯二甲酸丁二醇酯树脂组合物而进行了深入研究，结果发现，以末端羧基量为30meq/kg以下的聚对苯二甲酸丁二醇酯树脂为主体、向其中配混特定量的碳二亚胺化合物及根据需要配混一定量以下的弹性体而得到的组合物的耐热冲击性优异，并且能够维持高熔接强度，从而完成了本发明。
即，本发明为一种熔接用聚对苯二甲酸丁二醇酯树脂组合物，其中，
相对于100重量份(A)末端羧基量为30meq/kg以下的聚对苯二甲酸丁二醇酯树脂，配混以下成分而成：
(B)碳二亚胺化合物：设(A)聚对苯二甲酸丁二醇酯树脂的末端羧基量为1时，碳二亚胺官能团量为0.3～1.5当量的量
(C)弹性体：0～15重量份。
以及，将由上述聚对苯二甲酸丁二醇酯树脂组合物形成的成形品彼此通过热熔接接合而成的复合成形品、以及将由上述聚对苯二甲酸丁二醇酯树脂组合物形成的成形品与由其它材料形成的成形品通过热熔接接合而成的复合成形品。
根据本发明，可提供在冷热循环环境下高度的耐久性等性能和利用热熔接的接合加工性优异的熔接用聚对苯二甲酸丁二醇酯树脂组合物。本发明的熔接用聚对苯二甲酸丁二醇酯树脂组合物对于各种复合成形品、特别是嵌入有金属等的成形品是有用的。
附图说明
图1的(a)、(b)是表示在实施例中进行的激光熔接性试验中使用的试验片和试验方法的图。另外，图中的数值的单位为mm。
图2是表示实施例中进行的振动熔接性试验中使用的试验片的图。另外，图中的数值的单位为mm。
具体实施方式
以下，依次对本发明的树脂材料的构成成分进行详细说明。首先，作为本发明的树脂组合物的基础树脂的(A)聚对苯二甲酸丁二醇酯树脂是指：至少包含对苯二甲酸或其酯形成衍生物(低级醇酯等)的二羧酸成分与至少包含碳数4的亚烷基二醇(1，4-丁二醇)或其酯形成衍生物的二醇成分缩聚而获得的聚对苯二甲酸丁二醇酯树脂。聚对苯二甲酸丁二醇酯树脂并不限于均聚对苯二甲酸丁二醇酯树脂，也可以是含有60摩尔％以上(特别是75～95摩尔％左右)的对苯二甲酸丁二醇酯单元的共聚物。
本发明中，使用如下聚对苯二甲酸丁二醇酯树脂：将聚对苯二甲酸丁二醇酯树脂的粉碎试样在苄醇中、215℃下溶解10分钟，然后用0.01N的氢氧化钠水溶液滴定，测定的末端羧基量为30meq/kg以下，优选为25meq/kg以下。
使用末端羧基量超过30meq/kg的聚对苯二甲酸丁二醇酯树脂时，耐热冲击性的提高效果降低，此外在湿热环境下由于水解而导致强度降低变大。
此外，对末端羧基量的下限没有特别限定，但通常难以制造小于5meq/kg的聚对苯二甲酸丁二醇酯树脂，此外，小于5meq/kg的聚对苯二甲酸丁二醇酯树脂与碳二亚胺化合物的反应会不能充分进行，有可能耐热冲击性的提高效果不充分。因此，聚对苯二甲酸丁二醇酯树脂的末端羧基量优选为5meq/kg以上，特别优选为10meq/kg以上。
此外，理想的是，所使用的(A)聚对苯二甲酸丁二醇酯树脂的特性粘度(IV)为0.67～0.90dL/g。特性粘度超过0.90dL/g时，有时无法获得嵌入成形品所需的成形时的流动性。可以通过共混具有不同特性粘度的聚对苯二甲酸丁二醇酯树脂，例如通过共混特性粘度1.00dL/g与0.70dL/g的聚对苯二甲酸丁二醇酯树脂来实现0.90dL/g以下的特性粘度。另外，特性粘度例如可以在邻氯苯酚中、在温度35℃的条件下进行测定。
在聚对苯二甲酸丁二醇酯树脂中，作为除对苯二甲酸及其酯形成衍生物以外的二羧酸成分(共聚单体成分)，例如可例示出芳香族二羧酸成分(间苯二甲酸、邻苯二甲酸、萘二羧酸、二苯基醚二羧酸等C6～C12芳基二羧酸等)、脂肪族二羧酸成分(琥珀酸、己二酸、壬二酸、癸二酸等C4～C16烷基二羧酸、环己烷二羧酸等C5～C10环烷基二羧酸等)、或它们的酯形成衍生物等。这些二羧酸成分可以单独使用或组合两种以上使用。
优选的二羧酸成分(共聚单体成分)包括芳香族二羧酸成分(特别是间苯二甲酸等C6～C10芳基二羧酸)、脂肪族二羧酸成分(特别是己二酸、壬二酸、癸二酸等C6～C12烷基二羧酸)。
作为除1，4-丁二醇以外的二醇成分(共聚单体成分)，例如可列举出脂肪族二醇成分〔例如亚烷基二醇(乙二醇、丙二醇、三亚甲基二醇、1，3-丁二醇、六亚甲基二醇、新戊二醇、1，3-辛二醇等C2～C10亚烷基二醇、二乙二醇、三乙二醇、二丙二醇等聚氧化C2～C4亚烷基二醇等)、环己烷二甲醇、氢化双酚A等脂环式二醇等〕、芳香族二醇成分〔双酚A、4，4-二羟基联苯等芳香族醇、双酚A的C2～C4环氧烷烃加成物(例如双酚A的环氧乙烷2摩尔加成物、双酚A的环氧丙烷3摩尔加成物等)等〕、或它们的酯形成衍生物等。这些二醇成分也可以单独使用或组合两种以上使用。
优选的二醇成分(共聚单体成分)包括脂肪族二醇成分(特别是C2～C6亚烷基二醇、二乙二醇等聚氧化C2～C3亚烷基二醇、环己烷二甲醇等脂环式二醇)。
通过以前述化合物作为单体成分进行缩聚而生成的聚对苯二甲酸丁二醇酯聚合物均可以作为本发明的(A)成分使用。组合使用均聚对苯二甲酸丁二醇酯聚合物与聚对苯二甲酸丁二醇酯共聚物也是有用的。
在本发明中使用的(B)碳二亚胺化合物是指分子中具有碳二亚胺基(-N＝C＝N-)的化合物。作为碳二亚胺化合物，可以使用主链为脂肪族的脂肪族碳二亚胺化合物、主链为脂环族的脂环族碳二亚胺化合物、主链为芳香族的芳香族碳二亚胺化合物中的任意物质，从耐水解性的观点来看，优选使用芳香族碳二亚胺化合物。
作为脂肪族碳二亚胺化合物，可列举出二异丙基碳二亚胺、二辛基癸基碳二亚胺等，作为脂环族碳二亚胺化合物，可列举出二环己基碳二亚胺等。
作为芳香族碳二亚胺化合物，可列举出二苯基碳二亚胺、二-2，6-二甲基苯基碳二亚胺、N-甲苯甲酰基-N’-苯基碳二亚胺、二对硝基苯基碳二亚胺、二对氨基苯基碳二亚胺、二对羟基苯基碳二亚胺、二对氯苯基碳二亚胺、二对甲氧基苯基碳二亚胺、二-3，4-二氯苯基碳二亚胺、二-2，5-二氯苯基碳二亚胺、二邻氯苯基碳二亚胺、对亚苯基-双-二邻甲苯甲酰基碳二亚胺、对亚苯基-双-二环己基碳二亚胺、对亚苯基-双-二对氯苯基碳二亚胺、亚乙基-双-二苯基碳二亚胺等单碳二亚胺化合物或二碳二亚胺化合物及聚(4，4’-二苯基甲烷碳二亚胺)、聚(3，5’-二甲基-4，4’-联苯基甲烷碳二亚胺)、聚(对亚苯基碳二亚胺)、聚(间亚苯基碳二亚胺)、聚(3，5’-二甲基-4，4’-二苯基甲烷碳二亚胺)、聚(亚萘基碳二亚胺)、聚(1，3-二异丙基亚苯基碳二亚胺)、聚(1-甲基-3，5-二异丙基亚苯基碳二亚胺)、聚(1，3，5-三乙基亚苯基碳二亚胺)及聚(三异丙基亚苯基碳二亚胺)等聚碳二亚胺化合物，它们还可以组合使用两种以上。其中特别适用二-2，6-二甲基苯基碳二亚胺、聚(4，4’-二苯基甲烷碳二亚胺)、聚(亚苯基碳二亚胺)和聚(三异丙基亚苯基碳二亚胺)。
此外，优选的是，作为(B)碳二亚胺化合物，使用分子量为2000以上、优选为10000以上的碳二亚胺化合物。分子量小于2000时，在熔融混炼时、成形时停留时间长等情况下，有可能产生显著的气体、臭气。
关于(B)碳二亚胺化合物的配混量，在设(A)聚对苯二甲酸丁二醇酯树脂的末端羧基量为1时，碳二亚胺官能团量为0.3～1.5当量的量。
(B)成分过少时，无法获得作为本发明的目标的耐热冲击性改良效果。此外过多时，流动性降低，混合时、成形加工时容易引起凝胶成分、碳化物的生成，拉伸强度、弯曲强度等机械特性降低，或者在湿热下引起强度的急剧下降。这是由于，聚对苯二甲酸丁二醇酯树脂与无机填充剂的密合性被(B)成分阻碍。优选的配混量为碳二亚胺官能团量为0.5～1.5当量的量，更优选为0.8～1.2当量的量。
在本发明的聚对苯二甲酸丁二醇酯树脂组合物中可以配混(C)弹性体。理想的是，作为弹性体，为热塑性弹性体、核壳弹性体。作为热塑性弹性体，可列举出接枝化的烯烃系、苯乙烯系、聚酯系的弹性体。
(C)弹性体的添加量相对于100重量份(A)聚对苯二甲酸丁二醇酯树脂为15重量份以下，优选为1～10重量份，特别优选为5～10重量份。少于1重量份时，耐热冲击性改善效果小，多于15重量份时，熔接性变差。
作为接枝化的烯烃系弹性体，优选以乙烯和/或丙烯为主成分的共聚物，可以适用(a-1)乙烯-不饱和羧酸烷基酯共聚物或(a-2)由α-烯烃与α，β-不饱和酸的缩水甘油酯形成的烯烃系共聚物、和(b)主要为由下述通式(1)所示的重复单元构成的聚合物或共聚物中的一种或两种以上以支链或交联结构化学键合而成的接枝共聚物。
Figure BPA00001447636300081
(其中，R表示氢或低级烷基，X表示选自-COOCH3、-COOC2H5、-COOC4H9、-COOCH2CH(C2H5)C4H9、-C6H5、-CN中的一种或两种以上的基团)
所述接枝共聚物对耐热冲击性的改善特别有效。
作为(a-1)乙烯-不饱和羧酸烷基酯共聚物的具体例子，可列举出乙烯-丙烯酸共聚物、乙烯-甲基丙烯酸共聚物、乙烯-丙烯酸-丙烯酸乙酯共聚物、乙烯-丙烯酸乙酯共聚物、乙烯-醋酸乙烯酯共聚物、乙烯-醋酸乙烯酯-丙烯酸乙酯共聚物等无规共聚物，进一步可以将这些共聚物混合使用。另外，作为构成(a-2)的烯烃系共聚物一单体的α-烯烃，可列举出乙烯、丙烯、1-丁烯等，优选使用乙烯。此外，作为构成(a-2)成分的其它单体的α，β-不饱和酸的缩水甘油酯为下述通式(2)所示的化合物，例如可列举出丙烯酸缩水甘油酯、甲基丙烯酸缩水甘油酯、乙基丙烯酸缩水甘油酯等，特别优选使用甲基丙烯酸缩水甘油酯。
[化学式2]
Figure BPA00001447636300091
(其中，R1表示氢原子或低级烷基)
由α-烯烃(例如乙烯)与α，β-不饱和酸的缩水甘油酯形成的烯烃系共聚物可以通过通常熟知的自由基聚合反应进行共聚而获得。α-烯烃与α，β-不饱和酸的缩水甘油酯的比率为α-烯烃70～99重量％、α，β-不饱和酸的缩水甘油酯1～30重量％是合适的。
接着，与该烯烃系共聚物(a-1)或(a-2)接枝聚合的聚合物或共聚物(b)是指由前述通式(1)所示的重复单元的一种构成的均聚物或由两种以上构成的共聚物，例如可列举出聚甲基丙烯酸甲酯、聚丙烯酸乙酯、聚丙烯酸丁酯、聚丙烯酸-2乙基己酯、聚苯乙烯、聚丙烯腈、丙烯腈-苯乙烯共聚物、丙烯酸丁酯-甲基丙烯酸甲酯共聚物、丙烯酸丁酯-苯乙烯共聚物等，特别优选丙烯酸丁酯-甲基丙烯酸甲酯共聚物。这些聚合物或共聚物(b)也可以通过对应的乙烯基系单体的自由基聚合来制备。
本发明所优选使用的接枝共聚物并非单独使用所述(a-1)或(a-2)的烯烃系共聚物或(b)的(共)聚合物，为(a-1)或(a-2)的共聚物与(b)的(共)聚合物在至少一个位点具有化学键合的支链或交联结构的接枝共聚物时方始具有该特征，且通过具有所述接枝结构而获得单独配混(a-1)、(a-2)或(b)所无法获得的显著效果。这里，用于构成接枝共聚物的(a-1)或(a-2)与(b)的比例为95∶5～5∶95(重量比)、优选为80∶20～20∶80较佳。
接着，作为苯乙烯系弹性体，优选由聚苯乙烯嵌段和聚烯烃结构的弹性体嵌段构成的嵌段共聚物等。具体而言，可列举出苯乙烯-异戊二烯-苯乙烯嵌段共聚物(SIS)、苯乙烯-乙烯·丙烯-苯乙烯嵌段共聚物(SEPS)、苯乙烯-乙烯·丁烯-苯乙烯嵌段共聚物(SEBS)、苯乙烯-乙烯·乙烯/丙烯-苯乙烯嵌段共聚物(SEEPS)等。
接着，聚酯系弹性体可以分为聚醚型和聚酯型，只要其弯曲模量为1000MPa以下、优选为700MPa以下，则可以任意使用。弯曲模量超过1000Mpa时，得不到充分的柔软性。聚醚型是指以芳香族聚酯作为硬链段、以由氧化亚烷基二醇的聚合物和二羧酸形成的聚酯作为软链段的聚酯弹性体。硬链段中的芳香族聚酯单元是指二羧酸化合物与二羟基化合物的缩聚物、羟基羧酸化合物的缩聚物或者这三种成分化合物的缩聚物。例如可以使用聚对苯二甲酸丁二醇酯等作为硬链段。作为软链段，使用由聚亚烷基醚和二羧酸缩聚而得到的化合物。例如可以使用由四氢呋喃衍生的聚氧化四亚甲基二醇的酯化合物。上述聚醚弹性体市售的有例如东洋纺织株式会社制造的Perprene P-30B、P-70B、P-90B、P-280B，DU PONT-TORAY CO.，LTD.制造的Hytrel 4057、4767、6347、7247，Ticona公司制造的Riteflex 655等。
聚酯型是指以芳香族聚酯作为硬链段、以非晶性聚酯作为软链段的聚酯弹性体。硬链段中的芳香族聚酯单元与上述聚醚型同样。软链段是内酯的开环聚合物，即聚内酯、或由脂肪族二羧酸与脂肪族二醇衍生的脂肪族聚酯。作为聚酯型弹性体，例如市售的有东洋纺织株式会社制造的Perprene S-1002、S-2002等。
接着，核壳系弹性体是具有由核层(核部)和被覆该核层(核层的表面)的一部分或全部的壳层构成的多层结构的聚合物。核壳系弹性体优选核层由橡胶成分(软质成分)构成、特别优选由丙烯酸系橡胶构成。橡胶成分的玻璃化转变温度例如为低于0℃(例如-10℃以下)，优选为-20℃以下(例如-180～-25℃左右)，进一步优选为-30℃以下(例如-150～-40℃左右)。
作为橡胶成分的丙烯酸系橡胶是以丙烯酸系单体〔特别是丙烯酸烷基酯(丙烯酸丁酯等丙烯酸C1～C12烷基酯、优选为丙烯酸C1～C8烷基酯、进一步优选为丙烯酸C2～C6烷基酯)等丙烯酸酯〕为主成分的聚合物。丙烯酸系橡胶可以为丙烯酸系单体的均聚物或共聚物(丙烯酸系单体之间的共聚物、丙烯酸系单体与其它含不饱和键的单体的共聚物等)，也可以为丙烯酸系单体(及其他含不饱和键的单体)与交联制单体的共聚物。
本发明的聚对苯二甲酸丁二醇酯树脂组合物中可以进一步配混(D)无机填充剂。作为(D)无机填充剂，有纤维状填充剂和非纤维状填充剂，优选为纤维状填充剂。片状或粒状的非纤维状无机填充剂、例如玻璃珠、玻璃片、硅石、高岭土、滑石、粘土、硅灰石、氧化钛、氧化锌、氧化铝、碳酸钙、碳酸镁等单独使用时得不到充分的强度，所以优选与纤维状填充剂组合使用。
作为本发明中使用的纤维状填充剂，可列举出玻璃纤维、炭纤维、钛酸钾纤维、二氧化硅·氧化铝纤维、氧化锆纤维、金属纤维、有机纤维等，优选玻璃纤维。
作为玻璃纤维，优选使用公知的任意玻璃纤维，与玻璃纤维直径、圆筒、茧形剖面、椭圆剖面等形状、或者在短切原丝(chopped strand)、粗纱等的制造中使用时的长度、玻璃切割的方法无关。本发明中，对玻璃的种类也没有限定，从品质上考虑优选使用E玻璃、组成中含锆元素的耐腐蚀玻璃。
此外，本发明中，为了提高纤维状填充剂与树脂基体的界面特性，特别优选使用通过氨基硅烷化合物、环氧化合物等有机处理剂进行了表面处理的纤维状填充剂，特别优选使用以加热减量值表示的有机处理剂量为1重量％以上的玻璃纤维。作为所述纤维状填充剂中使用的氨基硅烷化合物、环氧化合物，可以优选使用公知的任意物质，不取决于在本发明中用于纤维状填充剂的表面处理的氨基硅烷化合物、环氧化合物的种类。
(D)无机填充剂相对于100重量份(A)聚对苯二甲酸丁二醇酯树脂使用10～100重量份。少于所述范围时，伴随冷热循环的线性膨胀变化大，在耐热冲击性上不优选。超过所述范围而配混时，材料的容许变形量降低，在耐热冲击性上不优选。优选为20～80重量份，特别优选为30～60重量份。
在本发明组合物中，为了根据其目的而进一步赋予所期望的特性，可以配混通常在热塑性树脂及热固化性树脂等中添加的公知的物质、即抗氧化剂、耐热稳定剂、紫外线吸收剂等稳定剂、抗静电剂、染料、颜料等着色剂、润滑剂、增塑剂及结晶化促进剂、结晶成核剂、环氧化合物等。
制备本发明中使用的树脂组合物可以使用作为现有的树脂组合物制备法通常使用的设备和方法而容易地制备。例如，1)将各成分混合后通过单螺杆或双螺杆的挤出机混炼挤出来制备颗粒，然后成形的方法，2)暂时制备组成不同的颗粒，将该颗粒以规定量混合供于成形而成形后得到目标组成的成形品的方法，3)向成形机中直接投入一种或两种以上各成分的方法等均可以使用。此外，从实现这些成分的均匀配混的方面来看，将树脂成分的一部分制成细粉体与其以外的成分混合添加的方法是优选的方法。
此外，(B)碳二亚胺化合物也可以以将树脂作为基体的母炼胶的形式配混，使用母炼胶在实际的处理方面还有很多方便之处。适宜使用利用聚对苯二甲酸丁二醇酯树脂形成的母炼胶，但也可以使用利用其它树脂制备成的母炼胶。利用聚对苯二甲酸丁二醇酯树脂的母炼胶时，只要调节至规定的配混量的范围内即可。母炼胶可以在熔融混炼时预先投入而制成均匀颗粒。此外，也可以将使除碳二亚胺化合物以外的成分预先通过熔融混炼等制成均匀颗粒并在成形时与碳二亚胺化合物的母炼胶颗粒干混而得到的颗粒共混品用于成形。
由本发明的聚对苯二甲酸丁二醇酯树脂组合物形成的成形品可以通过以激光熔接、振动熔接、超声波熔接、热板熔接、旋转熔接等为代表的热熔接加工方法来接合，保持高熔接强度并且在冷热循环环境下的耐久性优异，能够广泛利用于汽车领域、电气·电子领域等中。
本发明中，可以通过如上所述的热熔接将由上述聚对苯二甲酸丁二醇酯树脂组合物形成的成形品(A)与其它成形品(B)接合，从而制成复合成形品。在这种情况下，作为其它成形品(B)，可以是与由上述聚对苯二甲酸丁二醇酯树脂组合物形成的成形品(A)相同材料的成形品，也可以是由其它材料形成的成形品。
在由聚对苯二甲酸丁二醇酯树脂组合物形成的成形品为嵌入成形品的情况下，本发明的效果特别显著。
作为激光熔接、振动熔接、超声波熔接、热板熔接、旋转熔接等热熔接加工方法，可以直接应用以往公知的方法。在激光熔接的情况下，由上述聚对苯二甲酸丁二醇酯树脂组合物形成的成形品可以用于透过侧或吸收侧中的任一者，当然也可以用于两者。
通过热熔接将成形品(A)与其它成形品(B)接合时，可以在不损害本发明的效果的范围内，在成形品(A)与其它成形品(B)的接合面夹持衬垫、防水透湿片、薄膜、塑料透镜等功能部件。
实施例
以下通过实施例对本发明进一步详细说明，但本发明并不限定于这些实施例。
实施例1～7、比较例1～6
称量表1所示的成分后干混，使用
Figure BPA00001447636300141
的双螺杆挤出机(株式会社日本制钢所制造TEX-30)熔融混炼而制成颗粒(料筒温度260℃、排出量15kg/h、螺杆转速150rpm)。接着，由该颗粒制成各试验片，测定各种物性。将结果汇总示于表1中。
此外，所使用的成分的详细内容、物性评价的测定法如下所示。
(A)聚对苯二甲酸丁二醇酯树脂
·(A-1)聚对苯二甲酸丁二醇酯树脂：胜技高分子株式会社制造、特性粘度0.69、末端羧基量24meq/kg
·(A-2)二甲基间苯二甲酸(DMI)改性聚对苯二甲酸丁二醇酯树脂：在对苯二甲酸与1，4-丁二醇的反应中，使用12.5mol％的DMI代替对苯二甲酸的一部分(12.5mol％)作为共聚成分，制备改性聚对苯二甲酸丁二醇酯树脂。特性粘度0.76、末端羧基量25meq/kg
·(A-3)聚对苯二甲酸丁二醇酯树脂：胜技高分子株式会社制造、特性粘度0.70、末端羧基量45meq/kg
(B)碳二亚胺化合物
·(B-1)芳香族碳二亚胺化合物：Rhein Chemie Japan Ltd.，制造、Stabaxol P、分子量3000
·(B-2)芳香族碳二亚胺化合物：Rhein Chemie Japan Ltd.，制造、Stabaxol P400、分子量20000
(C)弹性体
·(C-1)NOF CORPORATION制造、MODIPER A5300(乙烯丙烯酸乙酯-接枝-丙烯酸丁酯/甲基丙烯酸甲酯)
·(C-2)株式会社可乐丽制造、SEPTON 4055(聚苯乙烯-聚(乙烯-乙烯/丙烯)嵌段·聚苯乙烯共聚物)
(D)玻璃纤维
·(D-1)日本电气硝子株式会社制造、ECS03-T127
[激光熔接性]
使用图1的(a)所示的试验片，对厚度1.5mmt圆板状试验片如图1的(b)所示照射940nm、照射直径
Figure BPA00001447636300151
输出功率30W的激光，将两试验片接合，测定破坏强度。
将底面切断后，使用ORIENTEC Co.，Ltd.制造的万能试验机UTA-50KN，以试验速度5mm/mm用
Figure BPA00001447636300152
的夹具冲压，测定破坏强度。
另外，作为上述试验片，厚度1.5mmt圆状试验片(X：透过侧)由上述颗粒成形，吸收侧试验片(Y)由在上述颗粒中配混有3重量％的黑色着色用炭黑(胜技高分子株式会社制造、商品名2020B)的物质成形。吸收侧试验片(Y)作为利用激光的发热体起作用。
[振动熔接性]
对于图2所示的两种圆筒状试验片，使用BRANSON公司制造的ORBITAL WELDER MODEL-100以起振振幅0.8mm、压力3bar、熔接量0.9mm进行熔接，测定破坏强度。
将底面切断后，使用ORIENTEC Co.，Ltd.制造的万能试验机UTA-50KN，以试验速度5mm/mm用
Figure BPA00001447636300153
的夹具冲压，测定破坏强度。
另外，上述圆筒状试验片均由上述颗粒成形而成。
[耐热冲击性]
使用颗粒，以树脂温度260℃、模具温度65℃、注射时间25秒、冷却时间10秒，在试验片成形用模具(在长22mm、宽22mm、高51mm的棱柱内部嵌入长18mm、宽18mm、高30mm的铁芯的模具)中嵌入注射成形，使一部分树脂部的最小壁厚达到1mm，制造了嵌入成形品。对所获得的嵌入成形品，使用冷热冲击试验机在140℃下加热1小时30分钟后，降温至-40℃冷却1小时30分钟，然后进一步升温至140℃，以这样的过程作为1个循环进行耐热冲击试验，测定直至成形品中有裂纹为止的循环数，评价耐热冲击性。
[表1]
Figure BPA00001447636300171

Claims (6)

1.一种熔接用聚对苯二甲酸丁二醇酯树脂组合物，其相对于100重量份(A)末端羧基量为30meq/kg以下的聚对苯二甲酸丁二醇酯树脂，配混以下成分而成：
(B)碳二亚胺化合物：设(A)聚对苯二甲酸丁二醇酯树脂的末端羧基量为1时，碳二亚胺官能团量为0.3～1.5当量的量；
(C)弹性体：0～15重量份。
2.根据权利要求1所述的熔接用聚对苯二甲酸丁二醇酯树脂组合物，其进一步配混相对于100重量份(A)聚对苯二甲酸丁二醇酯树脂为10～100重量份的(D)无机填充剂而成。
3.根据权利要求1或2所述的熔接用聚对苯二甲酸丁二醇酯树脂组合物，其中，(B)碳二亚胺化合物的分子量为2000以上。
4.一种复合成形品，其是将由权利要求1～3中的任一项所述的聚对苯二甲酸丁二醇酯树脂组合物形成的成形品彼此通过热熔接接合而成的。
5.一种复合成形品，其是将由权利要求1～3中的任一项所述的聚对苯二甲酸丁二醇酯树脂组合物形成的成形品与由其它材料形成的成形品通过热熔接接合而成的。
6.根据权利要求4或5所述的复合成形品，其中，由聚对苯二甲酸丁二醇酯树脂组合物形成的成形品为嵌入成形品。
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