CN103025790A - 粘接力改善用改性聚对苯二甲酸烷二醇酯树脂、粘接力改善用改性聚对苯二甲酸烷二醇酯树脂组合物、树脂成形体、接合体 - Google Patents
粘接力改善用改性聚对苯二甲酸烷二醇酯树脂、粘接力改善用改性聚对苯二甲酸烷二醇酯树脂组合物、树脂成形体、接合体 Download PDFInfo
- Publication number
- CN103025790A CN103025790A CN2011800362755A CN201180036275A CN103025790A CN 103025790 A CN103025790 A CN 103025790A CN 2011800362755 A CN2011800362755 A CN 2011800362755A CN 201180036275 A CN201180036275 A CN 201180036275A CN 103025790 A CN103025790 A CN 103025790A
- Authority
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- China
- Prior art keywords
- resin
- terephthalic acid
- terephthalate resin
- diol ester
- poly terephthalic
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
- Granted
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- 229920005989 resin Polymers 0.000 title claims abstract description 137
- 239000011347 resin Substances 0.000 title claims abstract description 137
- 229920001283 Polyalkylene terephthalate Polymers 0.000 title abstract 5
- 239000000853 adhesive Substances 0.000 title abstract 3
- 230000001070 adhesive effect Effects 0.000 title abstract 3
- 239000011342 resin composition Substances 0.000 title 1
- -1 polybutylene terephthalate Polymers 0.000 claims abstract description 76
- KKEYFWRCBNTPAC-UHFFFAOYSA-N Terephthalic acid Chemical compound OC(=O)C1=CC=C(C(O)=O)C=C1 KKEYFWRCBNTPAC-UHFFFAOYSA-N 0.000 claims abstract description 69
- 229920001707 polybutylene terephthalate Polymers 0.000 claims abstract description 32
- OFOBLEOULBTSOW-UHFFFAOYSA-N Malonic acid Chemical compound OC(=O)CC(O)=O OFOBLEOULBTSOW-UHFFFAOYSA-N 0.000 claims abstract description 30
- 125000003118 aryl group Chemical group 0.000 claims abstract description 14
- QQVIHTHCMHWDBS-UHFFFAOYSA-N isophthalic acid Chemical compound OC(=O)C1=CC=CC(C(O)=O)=C1 QQVIHTHCMHWDBS-UHFFFAOYSA-N 0.000 claims abstract description 7
- 239000003795 chemical substances by application Substances 0.000 claims description 52
- 238000012986 modification Methods 0.000 claims description 35
- 230000004048 modification Effects 0.000 claims description 35
- 239000000203 mixture Substances 0.000 claims description 22
- 150000007942 carboxylates Chemical class 0.000 claims description 16
- 238000000465 moulding Methods 0.000 claims description 15
- 238000007493 shaping process Methods 0.000 claims description 5
- 238000007334 copolymerization reaction Methods 0.000 claims description 4
- 238000000034 method Methods 0.000 abstract description 25
- 229920001296 polysiloxane Polymers 0.000 abstract description 3
- LYCAIKOWRPUZTN-UHFFFAOYSA-N Ethylene glycol Chemical compound OCCO LYCAIKOWRPUZTN-UHFFFAOYSA-N 0.000 description 11
- 238000004519 manufacturing process Methods 0.000 description 8
- 238000012360 testing method Methods 0.000 description 8
- 230000000694 effects Effects 0.000 description 6
- 239000004593 Epoxy Substances 0.000 description 5
- 230000000052 comparative effect Effects 0.000 description 5
- 150000002009 diols Chemical class 0.000 description 5
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- 230000000704 physical effect Effects 0.000 description 5
- MNAHQWDCXOHBHK-UHFFFAOYSA-N 1-phenylpropane-1,1-diol Chemical compound CCC(O)(O)C1=CC=CC=C1 MNAHQWDCXOHBHK-UHFFFAOYSA-N 0.000 description 4
- 229920001577 copolymer Polymers 0.000 description 4
- WGCNASOHLSPBMP-UHFFFAOYSA-N hydroxyacetaldehyde Natural products OCC=O WGCNASOHLSPBMP-UHFFFAOYSA-N 0.000 description 4
- QQVIHTHCMHWDBS-UHFFFAOYSA-L isophthalate(2-) Chemical compound [O-]C(=O)C1=CC=CC(C([O-])=O)=C1 QQVIHTHCMHWDBS-UHFFFAOYSA-L 0.000 description 4
- 230000000630 rising effect Effects 0.000 description 4
- 238000003466 welding Methods 0.000 description 4
- DNIAPMSPPWPWGF-UHFFFAOYSA-N Propylene glycol Chemical compound CC(O)CO DNIAPMSPPWPWGF-UHFFFAOYSA-N 0.000 description 3
- 125000003178 carboxy group Chemical group [H]OC(*)=O 0.000 description 3
- 150000001875 compounds Chemical class 0.000 description 3
- MTHSVFCYNBDYFN-UHFFFAOYSA-N diethylene glycol Chemical compound OCCOCCO MTHSVFCYNBDYFN-UHFFFAOYSA-N 0.000 description 3
- 150000002148 esters Chemical class 0.000 description 3
- 238000010438 heat treatment Methods 0.000 description 3
- 238000005304 joining Methods 0.000 description 3
- 239000000463 material Substances 0.000 description 3
- 229920000642 polymer Polymers 0.000 description 3
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- 239000002253 acid Substances 0.000 description 2
- 239000000654 additive Substances 0.000 description 2
- 230000000996 additive effect Effects 0.000 description 2
- 150000001335 aliphatic alkanes Chemical class 0.000 description 2
- 239000011248 coating agent Substances 0.000 description 2
- 238000000576 coating method Methods 0.000 description 2
- 230000006835 compression Effects 0.000 description 2
- 238000007906 compression Methods 0.000 description 2
- 238000005538 encapsulation Methods 0.000 description 2
- 229920006351 engineering plastic Polymers 0.000 description 2
- 125000004185 ester group Chemical group 0.000 description 2
- 239000007789 gas Substances 0.000 description 2
- 125000004435 hydrogen atom Chemical group [H]* 0.000 description 2
- 238000002347 injection Methods 0.000 description 2
- 239000007924 injection Substances 0.000 description 2
- 238000001746 injection moulding Methods 0.000 description 2
- 239000000178 monomer Substances 0.000 description 2
- BKIMMITUMNQMOS-UHFFFAOYSA-N nonane Chemical compound CCCCCCCCC BKIMMITUMNQMOS-UHFFFAOYSA-N 0.000 description 2
- 230000010412 perfusion Effects 0.000 description 2
- XNGIFLGASWRNHJ-UHFFFAOYSA-N phthalic acid Chemical compound OC(=O)C1=CC=CC=C1C(O)=O XNGIFLGASWRNHJ-UHFFFAOYSA-N 0.000 description 2
- 238000002360 preparation method Methods 0.000 description 2
- CXMXRPHRNRROMY-UHFFFAOYSA-N sebacic acid Chemical compound OC(=O)CCCCCCCCC(O)=O CXMXRPHRNRROMY-UHFFFAOYSA-N 0.000 description 2
- 239000000126 substance Substances 0.000 description 2
- PUPZLCDOIYMWBV-UHFFFAOYSA-N (1R)-1,3-butanediol Natural products CC(O)CCO PUPZLCDOIYMWBV-UHFFFAOYSA-N 0.000 description 1
- 229940058015 1,3-butylene glycol Drugs 0.000 description 1
- 239000004215 Carbon black (E152) Substances 0.000 description 1
- IAYPIBMASNFSPL-UHFFFAOYSA-N Ethylene oxide Chemical compound C1CO1 IAYPIBMASNFSPL-UHFFFAOYSA-N 0.000 description 1
- 238000012696 Interfacial polycondensation Methods 0.000 description 1
- GOOHAUXETOMSMM-UHFFFAOYSA-N Propylene oxide Chemical compound CC1CO1 GOOHAUXETOMSMM-UHFFFAOYSA-N 0.000 description 1
- BLRPTPMANUNPDV-UHFFFAOYSA-N Silane Chemical compound [SiH4] BLRPTPMANUNPDV-UHFFFAOYSA-N 0.000 description 1
- 239000004902 Softening Agent Substances 0.000 description 1
- ORLQHILJRHBSAY-UHFFFAOYSA-N [1-(hydroxymethyl)cyclohexyl]methanol Chemical compound OCC1(CO)CCCCC1 ORLQHILJRHBSAY-UHFFFAOYSA-N 0.000 description 1
- 238000007259 addition reaction Methods 0.000 description 1
- 239000002390 adhesive tape Substances 0.000 description 1
- 239000003963 antioxidant agent Substances 0.000 description 1
- 230000003078 antioxidant effect Effects 0.000 description 1
- IISBACLAFKSPIT-UHFFFAOYSA-N bisphenol A Chemical class C=1C=C(O)C=CC=1C(C)(C)C1=CC=C(O)C=C1 IISBACLAFKSPIT-UHFFFAOYSA-N 0.000 description 1
- 238000000071 blow moulding Methods 0.000 description 1
- 230000001680 brushing effect Effects 0.000 description 1
- 235000019437 butane-1,3-diol Nutrition 0.000 description 1
- WERYXYBDKMZEQL-UHFFFAOYSA-N butane-1,4-diol Chemical compound OCCCCO WERYXYBDKMZEQL-UHFFFAOYSA-N 0.000 description 1
- 239000003054 catalyst Substances 0.000 description 1
- 238000006757 chemical reactions by type Methods 0.000 description 1
- 238000006482 condensation reaction Methods 0.000 description 1
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- QYQADNCHXSEGJT-UHFFFAOYSA-N cyclohexane-1,1-dicarboxylate;hydron Chemical compound OC(=O)C1(C(O)=O)CCCCC1 QYQADNCHXSEGJT-UHFFFAOYSA-N 0.000 description 1
- 230000006837 decompression Effects 0.000 description 1
- 230000003247 decreasing effect Effects 0.000 description 1
- USIUVYZYUHIAEV-UHFFFAOYSA-N diphenyl ether Chemical compound C=1C=CC=CC=1OC1=CC=CC=C1 USIUVYZYUHIAEV-UHFFFAOYSA-N 0.000 description 1
- SZXQTJUDPRGNJN-UHFFFAOYSA-N dipropylene glycol Chemical compound OCCCOCCCO SZXQTJUDPRGNJN-UHFFFAOYSA-N 0.000 description 1
- 239000000428 dust Substances 0.000 description 1
- BXKDSDJJOVIHMX-UHFFFAOYSA-N edrophonium chloride Chemical compound [Cl-].CC[N+](C)(C)C1=CC=CC(O)=C1 BXKDSDJJOVIHMX-UHFFFAOYSA-N 0.000 description 1
- 125000003700 epoxy group Chemical group 0.000 description 1
- 229960005082 etohexadiol Drugs 0.000 description 1
- 238000001125 extrusion Methods 0.000 description 1
- 239000003063 flame retardant Substances 0.000 description 1
- 238000010528 free radical solution polymerization reaction Methods 0.000 description 1
- 239000003365 glass fiber Substances 0.000 description 1
- 150000002334 glycols Chemical class 0.000 description 1
- XXMIOPMDWAUFGU-UHFFFAOYSA-N hexane-1,6-diol Chemical compound OCCCCCCO XXMIOPMDWAUFGU-UHFFFAOYSA-N 0.000 description 1
- 229930195733 hydrocarbon Natural products 0.000 description 1
- 150000002430 hydrocarbons Chemical class 0.000 description 1
- 230000007062 hydrolysis Effects 0.000 description 1
- 238000006460 hydrolysis reaction Methods 0.000 description 1
- 230000005764 inhibitory process Effects 0.000 description 1
- 239000000314 lubricant Substances 0.000 description 1
- 238000005259 measurement Methods 0.000 description 1
- 239000000155 melt Substances 0.000 description 1
- 238000002844 melting Methods 0.000 description 1
- 230000008018 melting Effects 0.000 description 1
- 229910052751 metal Inorganic materials 0.000 description 1
- 239000002184 metal Substances 0.000 description 1
- SLCVBVWXLSEKPL-UHFFFAOYSA-N neopentyl glycol Chemical compound OCC(C)(C)CO SLCVBVWXLSEKPL-UHFFFAOYSA-N 0.000 description 1
- YZPOQCQXOSEMAZ-UHFFFAOYSA-N pbt2 Chemical class ClC1=CC(Cl)=C(O)C2=NC(CN(C)C)=CC=C21 YZPOQCQXOSEMAZ-UHFFFAOYSA-N 0.000 description 1
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical group [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 description 1
- 238000006068 polycondensation reaction Methods 0.000 description 1
- 229920001225 polyester resin Polymers 0.000 description 1
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- 238000003825 pressing Methods 0.000 description 1
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- 238000011160 research Methods 0.000 description 1
- 239000000523 sample Substances 0.000 description 1
- 229920006395 saturated elastomer Polymers 0.000 description 1
- 229910000077 silane Inorganic materials 0.000 description 1
- 229910052710 silicon Inorganic materials 0.000 description 1
- 239000002210 silicon-based material Substances 0.000 description 1
- 239000007787 solid Substances 0.000 description 1
- 125000003011 styrenyl group Chemical class [H]\C(*)=C(/[H])C1=C([H])C([H])=C([H])C([H])=C1[H] 0.000 description 1
- 238000006467 substitution reaction Methods 0.000 description 1
- 239000000758 substrate Substances 0.000 description 1
- 229920002725 thermoplastic elastomer Polymers 0.000 description 1
- 238000005809 transesterification reaction Methods 0.000 description 1
- ZIBGPFATKBEMQZ-UHFFFAOYSA-N triethylene glycol Chemical compound OCCOCCOCCO ZIBGPFATKBEMQZ-UHFFFAOYSA-N 0.000 description 1
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 1
Classifications
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Abstract
提供提高包含聚对苯二甲酸烷二醇酯树脂的树脂成形体对有机硅系粘接剂的粘接性的技术。使用如下聚对苯二甲酸烷二醇酯树脂:将除对苯二甲酸之外的芳香族二羧酸和/或其酯化物作为改性成分来共聚,相对于总二羧酸成分,上述改性成分的含量为13摩尔%以上且35摩尔%以下。改性聚对苯二甲酸烷二醇酯树脂优选为改性聚对苯二甲酸丁二醇酯树脂,芳香族二羧酸和/或其酯化物优选为间苯二甲酸和/或其酯化物。
Description
技术领域
本发明涉及:粘接力改善用改性聚对苯二甲酸烷二醇酯树脂、包含该树脂的树脂组合物、使该树脂组合物成形而成的树脂成形体、及将该树脂成形体与其它成形体接合而成的接合体。
背景技术
聚对苯二甲酸烷二醇酯树脂由于具有优异的机械强度、耐热性、电特性、成形性,因而作为工程塑料被利用于各种领域。
在聚对苯二甲酸烷二醇酯树脂中,聚对苯二甲酸丁二醇酯树脂具有特别优异的机械强度、电性质、其它物理、化学性质,并且加工性也优异。因此,聚对苯二甲酸丁二醇酯树脂作为工程塑料被用于汽车、电气·电子部件等广泛用途。
根据用途,需要接合多个树脂成形体。作为接合树脂成形体的方法,已知基于粘接剂的接合、双层成形、热板熔接、振动熔接、激光熔接等各种接合方法。接合方法的选择是考虑用途、树脂成形体的形状等来进行的,适当的接合方法根据用途而不同。另外,对于与其它树脂、金属的接合而言,熔接加工困难,因此通常采取粘接、螺纹紧固、铆接之类的手段。
例如,在用于减轻来自水分、粉尘、外部冲击等的损伤的、容纳搭载有电子部件的基板的外壳材料、配置有传感器探头、连接器端子等的嵌入成形品等的用途中,最为通常的是基于粘接剂的接合、基于灌注封装的保护。
作为粘接剂,可以使用环氧系粘接剂、有机硅系粘接剂等,但对于要求耐热性、耐寒性等的部件,优选使用有机硅系粘接剂。另外,已经在推进树脂成形体与有机硅系粘接剂的粘接性的改良,例如,已知改善包含聚对苯二甲酸丁二醇酯树脂的树脂成形体与有机硅系粘接剂的粘接强度的技术(专利文献1、2)。
例如,专利文献1中公开了与有机硅系粘接剂的粘接性良好的聚对苯二甲酸丁二醇酯树脂。另外,专利文献2中,公开了如下的方法:使聚对苯二甲酸丁二醇酯树脂组合物中含有特定的弹性体和玻璃纤维,由此改善树脂成形体与有机硅系粘接剂的粘接性。
近年来,正在研究树脂成形体对暴露于较以往更加严酷的环境中的用途的应用。在暴露于更加严酷的环境中时,需要进一步提高树脂成形体与有机硅系粘接剂的粘接性。
另外,已知有包含间苯二甲酸成分等单体作为共聚成分的改性聚对苯二甲酸丁二醇酯树脂(专利文献3、4)。专利文献3中公开了利用由结晶度降低导致的熔点降低,易于对其它构件进行熔接的技术。专利文献4中利用了抑制由结晶度降低导致的成形收缩时的变形的技术。
现有技术文献
专利文献
专利文献1:日本特开2001-040194号公报
专利文献2:国际公开WO2009/081572号小册子
专利文献3:日本特开2009-005911号公报
专利文献4:日本特开2009-155449号公报
发明内容
发明要解决的问题
本发明是为了解决以上问题而完成的,其目的在于,提供提高包含聚对苯二甲酸烷二醇酯树脂的树脂成形体对有机硅系粘接剂的粘接性的技术。
用于解决问题的方案
本发明人等为了解决上述问题而反复进行了深入研究。结果发现,使用将除对苯二甲酸之外的芳香族二羧酸和/或其酯化物作为改性成分来共聚、相对于总二羧酸成分的上述改性成分的含量为13摩尔%以上且35摩尔%以下的聚对苯二甲酸烷二醇酯树脂时,能够解决上述问题,进而完成了本发明。更具体而言,本发明提供以下的技术方案。
(1)一种粘接力改善用改性聚对苯二甲酸烷二醇酯树脂,将除对苯二甲酸之外的芳香族二羧酸和/或其酯化物作为改性成分来共聚,相对于总二羧酸成分,前述改性成分的含量为13摩尔%以上且35摩尔%以下。
(2)根据(1)所述的粘接力改善用改性聚对苯二甲酸烷二醇酯树脂,其中,前述改性聚对苯二甲酸烷二醇酯树脂为改性聚对苯二甲酸丁二醇酯树脂。
(3)根据(1)或(2)所述的粘接力改善用改性聚对苯二甲酸烷二醇酯树脂,其中,前述芳香族二羧酸和/或其酯化物为间苯二甲酸和/或其酯化物。
(4)一种树脂成形体,其是使(1)~(3)中的任一项所述的粘接力改善用改性聚对苯二甲酸烷二醇酯树脂组合物成形而成的。
(5)一种接合体,其为一对成形体介由有机硅粘接剂接合而成的接合体,前述一对成形体的至少一者为(4)所述的树脂成形体。
发明的效果
根据本发明,通过使用将除对苯二甲酸之外的芳香族二羧酸和/或其酯化物作为改性成分来共聚、相对于总二羧酸成分的上述改性成分的含量调整为13摩尔%以上且35摩尔%以下的改性聚对苯二甲酸烷二醇酯树脂,能够很大程度上改善树脂成形体与有机硅系粘接剂的粘接性。
具体实施方式
以下,对本发明的实施方式进行详细说明。需要说明的是,本发明不限定于以下的实施方式。
<粘接力改善用改性聚对苯二甲酸烷二醇酯树脂>
本发明的粘接力改善用改性聚对苯二甲酸烷二醇酯树脂(本说明书中有时称为“本发明的聚对苯二甲酸烷二醇酯树脂”)包含除对苯二甲酸之外的芳香族二羧酸和/或其酯化物作为改性成分,相对于总二羧酸成分,上述改性成分的含量为13摩尔%以上且35摩尔%以下。上述改性成分对高分子赋予弯曲结构。若对高分子赋予弯曲结构,则结晶度降低,有时机械强度等一部分物性也降低,但后述的与有机硅系粘接剂的粘接性大幅提高。
上述改性成分的含量为13摩尔%以上时,能够提高使用本发明的树脂而得到的树脂成形体对有机硅系粘接剂的粘接性,因而优选。上述改性成分的含量为35摩尔%以下时,能够抑制由结晶度降低导致的聚对苯二甲酸烷二醇酯树脂的物性降低,进而与未改性聚对苯二甲酸烷二醇酯的熔点差异小,因而使树脂成形时的固化充分且成形周期为适当的范围,因此在考虑生产率时也是优选的。对含量的上限,可以根据用途来适宜地进行设定。
本发明的聚对苯二甲酸烷二醇酯树脂是将二羧酸成分与包含烷二醇或其酯化物的二醇成分缩聚而得到的树脂。本发明的聚对苯二甲酸烷二醇酯树脂包含除对苯二甲酸之外的芳香族二羧酸和/或其酯化物(改性成分)作为二羧酸成分。这并不意味着将包含对苯二甲酸作为共聚成分的情况排除在外。即,本发明的树脂也包括如下的树脂:包含对苯二甲酸作为共聚成分、并且包含除对苯二甲酸之外的芳香族二羧酸和/或其酯化物作为共聚成分的树脂。
作为除对苯二甲酸之外的芳香族二羧酸和/或其酯化物,例如可列举出间苯二甲酸、邻苯二甲酸、2,6-萘二酸、4,4’-二羧基二苯醚等C8-14的芳香族二羧酸;琥珀酸、己二酸、壬二酸、癸二酸等C4-16的烷烃二羧酸;环己烷二羧酸等C5-10的环烷烃二羧酸;这些二羧酸成分的成酯性衍生物(C1-6的烷基酯衍生物、酰卤化物等)。这些二羧酸成分可以单独使用或组合使用两种以上。作为除对苯二甲酸之外的芳香族二羧酸和/或其酯化物(改性成分),特别优选使用间苯二甲酸和/或其酯化物。
作为二醇成分,可列举出例如1,4-丁二醇、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C2-10的亚烷基二醇;二乙二醇、三乙二醇、二丙二醇等多氧亚烷基二醇;环己烷二甲醇、氢化双酚A等脂环式二醇;双酚A、4,4’-二羟基联苯等芳香族二醇;双酚A的环氧乙烷2摩尔加成物、双酚A的环氧丙烷3摩尔加成物等的双酚A的C2-4的环氧烷加成物;或这些二醇的成酯性衍生物(乙酰化物等)。这些二醇成分可以单独使用或组合使用两种以上。
如上所述,可以使用各种二羧酸成分、二醇成分,但本发明中特别优选改性聚对苯二甲酸丁二醇酯树脂。改性聚对苯二甲酸丁二醇酯树脂是指,包含对苯二甲酸、除对苯二甲酸之外的芳香族二羧酸和/或其酯化物(改性成分)作为二羧酸成分,并且包含1,4-丁二醇作为二醇成分的树脂。
如上所述,对于改性聚对苯二甲酸丁二醇酯树脂,相对于总二羧酸成分,包含13摩尔%以上且35摩尔%以下的上述改性成分。如上所述,含有改性成分时结晶度降低,物性等有降低的倾向。然而,聚对苯二甲酸丁二醇酯树脂由于具有在聚对苯二甲酸烷二醇酯树脂中非常优异的物性,即使因上述结晶度低下导致物性有些降低,也能够对树脂成形体赋予非常优异的机械强度、电性质、其它物理、化学性质。另外,能够对得到的树脂成形体赋予与有机硅粘接剂的高粘接性。
另外,本发明的聚对苯二甲酸烷二醇酯树脂在不妨碍本发明的效果的范围内也可以含有除上述记载的单体之外的成分。
对于本发明的聚对苯二甲酸烷二醇酯树脂的末端羧基量,在不妨碍本发明的目的的范围内没有特别限制。本发明中使用的聚对苯二甲酸烷二醇酯树脂的末端羧基量优选为30meq/kg以下,更优选为25meq/kg以下。使用上述范围的末端羧基量的聚对苯二甲酸烷二醇酯树脂时,不易发生由湿热环境下的水解导致的强度降低。
另外,对于本发明的聚对苯二甲酸烷二醇酯树脂的熔体指数(MI),在不妨碍本发明的目的的范围内没有特别限制。上述熔体指数优选为5g/min以上且140g/min以下。进一步优选为20g/min以上且100g/min以下。使用上述范围的熔体指数的聚对苯二甲酸烷二醇酯树脂时,树脂组合物变得成形性特别优异。上述熔体指数是通过依据AS TM D-1238的方法、在235℃、载荷2160g的条件下测定的。需要说明的是,可以混合具有不同熔体指数的聚对苯二甲酸烷二醇酯树脂、其它树脂、其它成分(添加剂等)来调整熔体指数。
对于本发明的聚对苯二甲酸烷二醇酯树脂的结晶度,没有特别限定,但通常认为结晶度低是优选的。例如,推断通过以下数学式(I)算出时,优选为22%以下。存在上述改性成分的含量越多,高分子越容易成为弯曲结构的倾向。因此,结晶度可以通过调整改性成分的含量来进行调整。需要说明的是,结晶度采用通过使用以下数学式(I)的求出方法而得到的值时,结晶度成为22%以下时,明显地显示出提高与有机硅系粘接剂的粘接性的效果。
[数学式1]
结晶度(%)={ρc(ρ-ρa)/ρ(ρc-ρa)}×100 …(I)
(数学式(I)中的ρ为成为测定对象的树脂的密度、ρa为测定对象的树脂可视为结晶度0%时的密度、ρc为测定对象的树脂可视为结晶度100%时的密度。)
对本发明的聚对苯二甲酸烷二醇酯树脂的制造方法没有特别限定,但可以通过利用缩合反应、酯交换反应的界面缩聚、熔融聚合、溶液聚合等现有公知的方法来适宜地制造。另外,对得到的树脂在减压或非活性气体存在下进行热处理,使其固相聚合,从而能够进一步提高树脂的聚合度。
<粘接力改善用改性聚对苯二甲酸烷二醇酯树脂组合物>
本发明的粘接力改善用改性聚对苯二甲酸烷二醇酯树脂组合物(以下有时称为“本发明的树脂组合物”)包含上述粘接力改善用改性聚对苯二甲酸烷二醇酯树脂,也可以含有除改性聚对苯二甲酸烷二醇酯之外的用于提高与有机硅系粘接剂的粘接性的粘接性提高剂。对于粘接力改善用改性聚对苯二甲酸烷二醇酯树脂,与上述说明是同样的,因此省略说明。
[粘接性提高剂]
粘接性提高剂是指,除改性聚对苯二甲酸烷二醇酯之外的用于提高与有机硅粘接剂的粘接性的成分。例如,可列举出苯乙烯系热塑性弹性体、具有与硅原子键合的氢原子和三烷氧基甲硅烷基烷基的聚硅氧烷、具有丙烯酰氧基烷基的硅烷和有机过氧化物的组合、具有丙烯酰氧基烷基的硅氧烷和有机过氧化物的组合、硅原子上有环氧基和/或酯基以及硅原子上直接键合有氢原子的聚硅氧烷等含硅化合物。另外,除了这些化合物之外,作为提高与有机硅系粘接剂的粘接性的成分的现有公知的化合物、具有对提高与有机硅系粘接剂的粘接性做出贡献的结构的化合物也是粘接性提高剂。
[其它成分]
本发明的树脂组合物中,在不妨碍本发明的效果的范围内也可以含有其它树脂,另外,在不妨碍本发明的效果的范围内也可以含有成核剂、着色剂、抗氧化剂、稳定剂、增塑剂、润滑剂、脱模剂和阻燃剂等现有公知的添加剂。
[树脂组合物的制备]
上述本发明的树脂组合物可以使用一直以来用于制备树脂组合物的通常的设备、方法来容易地制备。
<树脂成形体>
本发明的树脂成形体是使上述本发明的树脂组合物成形而成的。本发明的成形体如后所述,与有机硅系粘接剂的粘接性优异。关于有机硅粘接剂,也在后面描述。
作为制造树脂成形体时的成形方法,可以采用现有公知的方法。作为现有公知的成形方法,例如可列举出注塑成形法、注塑压缩成形法、气体辅助注塑成形法、加热压缩成形法、挤出成形法、吹塑成形法等。
<接合体>
本发明的接合体是指,一对成形体介由有机硅粘接剂接合而成的接合体,上述一对成形体的至少一者为本发明的树脂成形体。本发明的树脂成形体由于与有机硅系粘接剂的粘接性优异,因而本发明的树脂成形体与有机硅系粘接剂粘接的部位几乎不产生粘接不良的问题。
另外,使一对成形体的两者均为本发明的树脂成形体时,任一成形体与有机硅系粘接剂的粘接性都高,因此不易产生粘接不良的问题。另外,两个成形体与有机硅系粘接剂的粘接性都高,因此一对成形体接合得更牢固。
有机硅系粘接剂是通过室温或加热来固化的粘接剂,可以使用现有公知的粘接剂,特别优选使用通过基于铂系催化剂的加成反应来进行固化的加成反应型有机硅粘接剂。
接着,对接合体的制造方法进行说明。对接合体的制造方法没有特别限定,例如可以通过如下的方法来制造。
此处,对接合第一树脂成形体与第二树脂成形体的情况进行说明。被接合的成形体的数目可以是两个以上。
首先,在第一树脂成形体上配置有机硅系粘接剂。对配置方法没有特别限定,例如可列举出刷涂、灌注封装等方法。接着,将第二树脂成形体载置在配置于第一树脂成形体上的有机硅系粘接剂上,根据需要在第一树脂成形体与第二树脂成形体重叠的方向上施加压力,从而使第一树脂成形体与第二树脂成形体密合。最后,通过室温或加热来使有机硅系粘接剂固化。
[实施例]
以下示出实施例和比较例,具体说明本发明,但本发明不限定于这些实施例。
<材料>
未改性聚对苯二甲酸丁二醇酯树脂1(未改性PB T1):宝理塑料株式会社制造,商品名“DURANEX400FP”(熔体指数(MI):45g/10min)
未改性聚对苯二甲酸丁二醇酯树脂2(未改性PB T2):宝理塑料株式会社制造,商品名“DURANEX500FP”(熔体指数(MI):20g/10min)
需要说明的是,熔体指数是通过依据AS TM D-1238的方法、在235℃、载荷2160g的条件下测定的。
改性聚对苯二甲酸丁二醇酯树脂1(改性PB T1):12.5摩尔%间苯二甲酸改性聚对苯二甲酸丁二醇酯(熔体指数(MI):46g/10min)
改性聚对苯二甲酸丁二醇酯树脂2(改性PBT2):15摩尔%间苯二甲酸改性聚对苯二甲酸丁二醇酯(熔体指数(MI):46g/10min)
改性聚对苯二甲酸丁二醇酯树脂3(改性PBT3):17摩尔%间苯二甲酸改性聚对苯二甲酸丁二醇酯(熔体指数(MI):30g/10min)
改性聚对苯二甲酸丁二醇酯树脂4(改性PBT4):30摩尔%间苯二甲酸改性聚对苯二甲酸丁二醇酯(熔体指数(MI):46g/10min)
[粘接剂]
有机硅系粘接剂:Dow Corning Toray Co.,Ltd.制造,商品名“SE1714”
环氧系粘接剂:Nagase Chemtex Corporation制造,商品名“XNR3503”
<树脂成形体的制造>
将未改性聚对苯二甲酸丁二醇酯树脂1、2和改性聚对苯二甲酸丁二醇酯树脂1~4分别投入到注塑成形机(FANUC公司制造的S2000i100B)中,制作用于后述的粘接强度测定的树脂试验片(依据ISO3167的多用途试验片)。得到实施例1~3的树脂成形体、比较例1~3的树脂成形体。
<接合体的制作>
裁切依据IS O3167的多用途试验片的中央部,在一片树脂试验片上粘附7mm×7mm开孔的日东电工株式会社制造的NITOFLON粘合带(厚度0.18mm),在孔的部分涂布有机硅系粘接剂。涂布后,重叠另一片树脂试验片,用夹具固定,在120℃×1小时的条件下进行粘接。得到使用有机硅系粘接剂来制作的实施例1~3接合体和比较例1~3的接合体。
将有机硅系粘接剂改变为环氧系粘接剂,将固化条件改变为120℃×0.5小时,除此之外通过与上述接合体同样的方法来制造接合体。得到使用环氧系粘接剂来制作的实施例1~3接合体和比较例1~3的接合体。
<粘接强度的测定>
将接合体在23℃、50%RH的环境下放置24小时以上,使用ORIENTEC制造的万能试验机TENSILON RTC-1325PL、在按压剥离试验速度5mm/min的条件下将粘接好的另一片树脂试验片按压剥离,测定按压剥离强度的最高值。将测定结果示于表1。
<结晶度的测定>
测定未改性聚对苯二甲酸丁二醇酯树脂1、2和改性聚对苯二甲酸丁二醇酯树脂1~4的各树脂的结晶度作为参考值。各树脂的密度通过水中置换法(依据JIS K7112)来测定。依照上述数学式(I),通过饱和聚酯树脂手册(日刊工业新闻社),在聚对苯二甲酸丁二醇酯的结晶密度ρc=1.40、非晶密度ρa=1.28的条件下计算出结晶度。
[表1]
由实施例、比较例的结果显然可以确认,改性成分的含量为13摩尔%以上,有机硅粘接强度得到提高。
由实施例的结果,使用有机硅系粘接剂时,显然可以确认到提高上述接合体的粘接强度的效果。确认到,使用环氧系粘接剂时,即使是改性PBT,也只有与未改性PBT同等的粘接强度。
由实施例的结果显然可以确认,改性成分的含量越多、结晶度越低的树脂越能提高有机硅粘接强度。
Claims (5)
1.一种粘接力改善用改性聚对苯二甲酸烷二醇酯树脂,其中,将除对苯二甲酸之外的芳香族二羧酸和/或其酯化物作为改性成分来共聚,
相对于总二羧酸成分,所述改性成分的含量为13摩尔%以上且35摩尔%以下。
2.根据权利要求1所述的粘接力改善用改性聚对苯二甲酸烷二醇酯树脂,其中,所述改性聚对苯二甲酸烷二醇酯树脂为改性聚对苯二甲酸丁二醇酯树脂。
3.根据权利要求1或2所述的粘接力改善用改性聚对苯二甲酸烷二醇酯树脂,其中,所述芳香族二羧酸和/或其酯化物为间苯二甲酸和/或其酯化物。
4.一种树脂成形体,其是使权利要求1~3中的任一项所述的粘接力改善用改性聚对苯二甲酸烷二醇酯树脂组合物成形而成的。
5.一种接合体,其为一对成形体介由有机硅粘接剂接合而成的接合体,
所述一对成形体的至少一者为权利要求4所述的树脂成形体。
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- 2011-05-31 US US13/702,885 patent/US11124602B2/en active Active
- 2011-05-31 MY MYPI2012005308A patent/MY160890A/en unknown
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JPWO2011155366A1 (ja) | 2013-08-01 |
US20130177774A1 (en) | 2013-07-11 |
MY160890A (en) | 2017-03-31 |
JP5744018B2 (ja) | 2015-07-01 |
US11124602B2 (en) | 2021-09-21 |
CN103025790B (zh) | 2014-12-03 |
WO2011155366A1 (ja) | 2011-12-15 |
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