CN1541250A - 含有abs的复合材料 - Google Patents
含有abs的复合材料 Download PDFInfo
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- CN1541250A CN1541250A CNA028156374A CN02815637A CN1541250A CN 1541250 A CN1541250 A CN 1541250A CN A028156374 A CNA028156374 A CN A028156374A CN 02815637 A CN02815637 A CN 02815637A CN 1541250 A CN1541250 A CN 1541250A
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- vinylbenzene
- polymerization
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- 239000002131 composite material Substances 0.000 title description 2
- 239000000463 material Substances 0.000 claims abstract description 17
- 229920000642 polymer Polymers 0.000 claims abstract description 14
- ISWSIDIOOBJBQZ-UHFFFAOYSA-N Phenol Chemical compound OC1=CC=CC=C1 ISWSIDIOOBJBQZ-UHFFFAOYSA-N 0.000 claims abstract description 5
- 229910052751 metal Inorganic materials 0.000 claims abstract description 5
- 239000002184 metal Substances 0.000 claims abstract description 5
- 229920003023 plastic Polymers 0.000 claims abstract description 5
- 239000004033 plastic Substances 0.000 claims abstract description 5
- 239000011159 matrix material Substances 0.000 claims description 27
- PPBRXRYQALVLMV-UHFFFAOYSA-N Styrene Chemical compound C=CC1=CC=CC=C1 PPBRXRYQALVLMV-UHFFFAOYSA-N 0.000 claims description 22
- 239000000203 mixture Substances 0.000 claims description 21
- -1 N-substituted maleimide amine Chemical class 0.000 claims description 15
- NLHHRLWOUZZQLW-UHFFFAOYSA-N Acrylonitrile Chemical compound C=CC#N NLHHRLWOUZZQLW-UHFFFAOYSA-N 0.000 claims description 14
- 239000000178 monomer Substances 0.000 claims description 14
- 229920001971 elastomer Polymers 0.000 claims description 13
- 239000005060 rubber Substances 0.000 claims description 13
- 238000010528 free radical solution polymerization reaction Methods 0.000 claims description 12
- 238000012662 bulk polymerization Methods 0.000 claims description 10
- 238000010557 suspension polymerization reaction Methods 0.000 claims description 10
- VVQNEPGJFQJSBK-UHFFFAOYSA-N Methyl methacrylate Chemical compound COC(=O)C(C)=C VVQNEPGJFQJSBK-UHFFFAOYSA-N 0.000 claims description 9
- XYLMUPLGERFSHI-UHFFFAOYSA-N alpha-Methylstyrene Chemical compound CC(=C)C1=CC=CC=C1 XYLMUPLGERFSHI-UHFFFAOYSA-N 0.000 claims description 9
- 238000006116 polymerization reaction Methods 0.000 claims description 9
- 238000002360 preparation method Methods 0.000 claims description 9
- 239000000725 suspension Substances 0.000 claims description 9
- 229920000578 graft copolymer Polymers 0.000 claims description 8
- FPYJFEHAWHCUMM-UHFFFAOYSA-N maleic anhydride Chemical compound O=C1OC(=O)C=C1 FPYJFEHAWHCUMM-UHFFFAOYSA-N 0.000 claims description 8
- GYCMBHHDWRMZGG-UHFFFAOYSA-N Methylacrylonitrile Chemical compound CC(=C)C#N GYCMBHHDWRMZGG-UHFFFAOYSA-N 0.000 claims description 7
- 238000010559 graft polymerization reaction Methods 0.000 claims description 6
- 229920005989 resin Polymers 0.000 claims description 6
- 239000011347 resin Substances 0.000 claims description 6
- 239000000126 substance Substances 0.000 claims description 4
- 229920005992 thermoplastic resin Polymers 0.000 claims description 4
- 239000004698 Polyethylene Substances 0.000 claims description 3
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 claims description 3
- 150000001408 amides Chemical class 0.000 claims description 3
- 229920000573 polyethylene Polymers 0.000 claims description 3
- 230000007704 transition Effects 0.000 claims description 3
- 239000004593 Epoxy Substances 0.000 claims description 2
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- 229910000831 Steel Inorganic materials 0.000 claims description 2
- 229920005822 acrylic binder Polymers 0.000 claims description 2
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- 125000000217 alkyl group Chemical group 0.000 abstract 1
- 125000002887 hydroxy group Chemical group [H]O* 0.000 abstract 1
- 150000002739 metals Chemical class 0.000 abstract 1
- 238000000034 method Methods 0.000 description 7
- KAKZBPTYRLMSJV-UHFFFAOYSA-N Butadiene Chemical group C=CC=C KAKZBPTYRLMSJV-UHFFFAOYSA-N 0.000 description 6
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- JLBJTVDPSNHSKJ-UHFFFAOYSA-N 4-Methylstyrene Chemical compound CC1=CC=C(C=C)C=C1 JLBJTVDPSNHSKJ-UHFFFAOYSA-N 0.000 description 1
- 229920003319 Araldite® Polymers 0.000 description 1
- 239000004610 Internal Lubricant Substances 0.000 description 1
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- NSOXQYCFHDMMGV-UHFFFAOYSA-N Tetrakis(2-hydroxypropyl)ethylenediamine Chemical compound CC(O)CN(CC(C)O)CCN(CC(C)O)CC(C)O NSOXQYCFHDMMGV-UHFFFAOYSA-N 0.000 description 1
- 239000002253 acid Substances 0.000 description 1
- 230000000996 additive effect Effects 0.000 description 1
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- 230000001070 adhesive effect Effects 0.000 description 1
- KKEYFWRCBNTPAC-UHFFFAOYSA-N benzene-dicarboxylic acid Natural products OC(=O)C1=CC=C(C(O)=O)C=C1 KKEYFWRCBNTPAC-UHFFFAOYSA-N 0.000 description 1
- MTAZNLWOLGHBHU-UHFFFAOYSA-N butadiene-styrene rubber Chemical compound C=CC=C.C=CC1=CC=CC=C1 MTAZNLWOLGHBHU-UHFFFAOYSA-N 0.000 description 1
- 238000006243 chemical reaction Methods 0.000 description 1
- 239000000470 constituent Substances 0.000 description 1
- 229920001577 copolymer Polymers 0.000 description 1
- 238000007334 copolymerization reaction Methods 0.000 description 1
- OMFXVFTZEKFJBZ-HJTSIMOOSA-N corticosterone Chemical compound O=C1CC[C@]2(C)[C@H]3[C@@H](O)C[C@](C)([C@H](CC4)C(=O)CO)[C@@H]4[C@@H]3CCC2=C1 OMFXVFTZEKFJBZ-HJTSIMOOSA-N 0.000 description 1
- 238000007720 emulsion polymerization reaction Methods 0.000 description 1
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- 239000000945 filler Substances 0.000 description 1
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- 238000005469 granulation Methods 0.000 description 1
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- 238000007254 oxidation reaction Methods 0.000 description 1
- 239000008188 pellet Substances 0.000 description 1
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- 230000003068 static effect Effects 0.000 description 1
- 239000003351 stiffener Substances 0.000 description 1
- 239000011115 styrene butadiene Substances 0.000 description 1
- 229920003048 styrene butadiene rubber Polymers 0.000 description 1
- 150000003440 styrenes Chemical class 0.000 description 1
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Abstract
本发明涉及包含下列组分的复合材料：I)ABS组分，包括：A)ABS聚合物和B)0.05－5wt％至少一种包含至少一个空间位阻羟基基团的酚，所述基团选自通式(I)－(IV)的结构单元，其中R代表C10－C18烷基；II)至少一种选自金属、其它塑料或其它材料的另外的材料。
Description
本发明涉及含有ABS组分和至少一种其它材料的复合材料以及可由该复合材料获得的模制品。
ABS型聚合物为两相塑料，包括：
1)形成树脂的单体，例如苯乙烯和丙烯腈的热塑性共聚物形成外部相，其中苯乙烯可以部分或全部被α-甲基苯乙烯或甲基丙烯酸甲酯替代，该共聚物亦被称作SAN树脂或基体树脂；
2)通过1)中所述的一种或多种单体在丁二烯均聚物或共聚物(接枝基体)上的接枝反应而制备的至少一种接枝聚合物。该接枝聚合物(“弹性体相”或“接枝橡胶”)在基体树脂中形成分散相。
ABS聚合物1)和2)可以通过已知的方法如乳液、溶液、本体、悬浮或沉淀聚合方法或者通过这些方法的组合方法进行制备。
如果复合材料是通过这些ABS聚合物特别是ABS聚合物粘合而制备的，且其中组分1)和2)的至少一种是通过本体或溶液聚合方法制备的，则会得到不充足的粘合性能或不希望的粘合层的分离。
因此本发明的目的是提供包括ABS组分和至少一种其它材料的复合材料，其不显示不充足的粘合性能。
现已令人惊讶地发现，本目的可通过包含规定量的空间位阻酚的ABS聚合物来实现。
因此本发明涉及包含下列组分的复合材料：
I)ABS组分，包括：
A)ABS聚合物和
B)相对I)占0.05-5wt％，优选0.1-4wt％，最优选0.5-3wt％的至少一种包含至少一个空间位阻羟基基团的酚，所述基团选自通式(I)-(IV)的结构单元：
其中R代表C10-C18烷基，并且还包含
II)至少一种其它材料，选自金属，优选铝或钢，其它塑料，优选聚氯乙烯、聚对苯二甲酸亚烷基二酯、聚碳酸酯、聚酰胺或聚烯烃或其混合物，最优选聚乙烯和聚丙烯，以及其它材料，优选木材。
A)中定义的ABS聚合物包括：
A.1)5-100wt％，优选7.5-80wt％，最优选10-70wt％至少一种通过溶液、悬浮或本体聚合获得的接枝聚合物，或者5-80wt％，优选7.5-70wt％，最优选10-60wt％至少一种通过乳液聚合获得的接枝聚合物，和
A.2)95-0wt％，优选92.5-20wt％，最优选90-30wt％(当使用通过溶液、悬浮或本体聚合获得的接枝聚合物时)，或95-20wt％，优选92.5-30wt％，最优选90-40wt％(当使用通过乳液聚合获得的接枝聚合物时)至少一种热塑性树脂。
本发明意义上的接枝聚合物为，选自丙烯腈、甲基丙烯腈、马来酸酐、N-取代马来酰亚胺、苯乙烯、α-甲基苯乙烯、包含取代环的苯乙烯或甲基丙烯酸甲酯的单体或单体混合物接枝聚合到橡胶(接枝基体)上的那些。
适宜的橡胶实际上包括所有玻璃化转变温度≤10℃的橡胶，优选包含通过聚合引入的丁二烯的橡胶。实例包括聚丁二烯、苯乙烯-丁二烯聚合物、丙烯腈-丁二烯聚合物、丙烯酸类橡胶(任选包含由丁二烯衍生引入的结构单元)、丙烯酸酯橡胶(包含，作为其芯，交联的橡胶如聚丁二烯或丁二烯与烯键式不饱和单体如苯乙烯和/或丙烯腈的共聚物)。聚丁二烯是优选的。
接枝聚合物包含3-95wt％，特别是5-70wt％的橡胶，和97-5wt％，特别是95-30wt％的接枝共聚单体。在这些接枝聚合物中，橡胶以至少部分交联的微粒形式存在，微粒的平均粒径(d50)为0.05-20.0μm，最优选为0.1-0.8μm，其中平均粒径d50可以通过超离心测量法测定(见W.Scholtan，H.Lange：Kolloid.-Z.und Z.Polymere250(1972)，782-796)。
适宜的制备方法包括乳液、溶液、本体或悬浮聚合路线；通过乳液聚合和/或溶液或本体聚合制备的接枝聚合物A)是特别优选的。
热塑性聚合物A.2)可以由接枝聚合在橡胶上的单体(接枝单体)或类似的单体制备，特别是由选自苯乙烯、α-甲基苯乙烯、对甲基苯乙烯、卤代苯乙烯、丙烯腈、甲基丙烯腈、甲基丙烯酸甲酯、马来酸酐、N-取代马来酰亚胺、特别是N-苯基马来酰亚胺的至少两种单体或其混合物制备。
优选的热塑性树脂A.2)优选为可由95-50wt％苯乙烯、α-甲基苯乙烯或甲基丙烯酸甲酯或其混合物和5-50wt％丙烯腈、甲基丙烯腈、甲基丙烯酸甲酯或马来酸酐或其混合物获得的共聚物。
特别优选的热塑性共聚物包含20-40wt％丙烯腈和80-60wt％苯乙烯或α-甲基苯乙烯，它们是通过聚合引入的。这些共聚物是已知的。优选其分子量(Mw)为15,000-200,000(由凝胶渗透色谱(GPC)测定)。
热塑性聚合物A.2)优选由溶液或本体聚合制备。
特别优选的ABS聚合物A)由下列物质A.1.1和A.1.2合成：
A.1.15-100wt％至少一种通过溶液、悬浮或本体聚合获得的接枝共聚物，或5-80wt％至少一种通过乳液聚合获得的接枝共聚物，其中每种共聚物都是通过使下列1.1的单体混合物在1.2上进行接枝聚合而制备的，
1.15-97wt％下列单体的混合物
1.1.15-50wt％丙烯腈、甲基丙烯腈、马来酸酐、N-取代马来酰亚胺或其混合物，和
1.1.295-50wt％苯乙烯、α-甲基苯乙烯、包含取代环的苯乙烯、甲基丙烯酸甲酯或其混合物，
1.295-3wt％至少一种玻璃化转变温度TG＜10℃的橡胶，
A.1.20-95wt％(当使用通过溶液、悬浮或本体聚合获得的接枝共聚物时)或20-95wt％(当使用通过乳液聚合获得的接枝共聚物时)至少一种热塑性树脂，其是通过溶液、悬浮或本体聚合由下列单体制备的：
2.15-50wt％丙烯腈、甲基丙烯腈、马来酸酐、N-取代马来酰亚胺或其混合物，和
2.295-50wt％苯乙烯、α-甲基苯乙烯、包含取代环的苯乙烯、甲基丙烯酸甲酯或其混合物。
组分B)限定的包含至少一个空间位阻羟基基团的化合物是已知的或者可通过已知方法制备。适宜化合物B)的实例包括下式(V)-(XXV)的化合物，它们均是已知的抗氧剂。
式(V)和(XIX)的化合物是特别优选的，并且是分别以商品名Irganox1076和Irganox245出售的。
这些化合物在高温，例如100-300℃于常规的混合装置、捏合机、密炼机、圆筒研磨机、连续螺杆挤出机或挤出机中与上述ABS聚合物混合。混合过程所用的停留时间可根据所要求的混合强度在10秒至30分钟之间变化。
除了根据本发明所用的化合物外，可以将常规添加剂如颜料、填料、稳定剂、抗静电剂、内润滑剂、脱模剂、阻燃剂等加入到ABS组分中。
优选ABS组分通过粘合与其它材料结合在一起形成根据本发明的复合材料。本领域技术人员已知的用于粘合复合材料的粘合剂适用于此目的。环氧树脂和丙烯酸酯粘合剂是特别优选的。
根据本发明的复合材料适于制造模制品、片材和板条。
这类模制品的实例包括由自两层或多层，例如金属和塑料层构成的片材或板条组成的层合材料。
实施例
所有的份均以重量份给出。
1.所用组分
A.1)包含50wt％平均粒径(d50)为0.35μm的聚丁二烯的接枝橡胶，在乳液中其上接枝聚合上36.5wt％苯乙烯和13.5wt％丙烯腈。
A.2)包含50wt％平均粒径(d50)为0.1μm的聚丁二烯的接枝橡胶，在乳液中其上接枝聚合上36.5wt％苯乙烯和13.5wt％丙烯腈。
A.3)苯乙烯/丙烯腈(SAN)为72∶28的、平均分子量(Mw)为约85,000的、通过溶液聚合制备的共聚物。
A.4)苯乙烯/丙烯腈(SAN)为72∶28的、平均分子量(Mw)为约85,000的、通过乳液聚合制备的共聚物。
B.1)Irganox1076(Ciba，巴塞尔，瑞士)
B.2)Irganox245(Ciba，巴塞尔，瑞士)
C.1)聚乙烯醇(Mowiol26-88，Hoechst AG)
C.2)树脂酸混合物的钠盐(Dresinate731的钠盐，AbietaChemie GmbH，Gersthofen)
C.3)马来酸酐
2.模塑组合物的制备及试验
将表1中所列各聚合物组分(重量份)与亦在表1中列出的添加剂及0.5重量份乙二胺二硬脂酰胺在密炼机(internal kneader)中于200-230℃混合3-5分钟，并随后进行造粒。
在195℃对粒料进行压制形成厚约0.5mm的板条。然后将由其切割而来的薄片使用双组分粘合剂(AralditeAW 136H，由瑞士巴塞尔的Ciba供应，硬化剂HY 994由瑞士巴塞尔的Ciba供应)一面粘合到铝片(约1mm厚)上而另一面粘合到聚乙烯薄膜上。当薄片-薄膜复合材料粘合到一起后，将其在100℃下压制(10t载荷下)固化20分钟，然后在保持相同加压载荷下冷却至室温。
粘合剂固化后2天进行手工测试测定粘合强度，采用下列评级体系：
+：复合材料不能手工分离(粘合良好)
0：复合材料可部分手工分离(粘合不良)
-：复合材料易于手工分离(未粘合)
亦在表1给出的粘合强度试验的评定结果说明，当将根据本发明的ABS聚合物粘合到金属和聚烯烃上时显示出很好的粘合性。
表1 ABS聚合物的组成及由其制备的
复合材料的试验结果(粘合强度)
实施例 A.1 A.2 A.3 A.4 B.1 B.2 C.1 C.2 C.3 手工测试的
粘结强度
(以重量份计的数据)
1 35.5 33.5 33 - 2 - - - - +
2 33.5 33.5 33 - - 2.5 - - - +
3(对比例) 33.5 33.5 33 - - - 2 - - -
4(对比例) 33.5 33.5 33 - - - - 2 - -
5(对比例) 33.5 33.5 33 - - - - - 2 0
6(对比例) 33.5 33.5 33 - - - - - - -
7(对比例) 33.5 33.5 - 33 - - - - - 0
8 33.5 33.5 - 33 1.5 - - - - +
Claims (10)
1.复合材料，包括：
I)ABS组分，包括：
A)ABS聚合物和
B)0.05-5wt％至少一种包含至少一个空间位阻羟基基团的酚，所述基团选自通式(I)-(IV)的结构单元：
其中R代表C10-C18烷基，并且还包括
II)至少一种选自金属、其它塑料以及其它材料的另外的材料。
2.根据权利要求1的复合材料，其中ABS聚合物A)由下述物质组成：
1.5-100wt％至少一种通过溶液、悬浮或本体聚合获得的接枝共聚物，或5-80wt％至少一种通过乳液聚合获得的接枝共聚物，其中每种共聚物都是通过使下列1.1的单体混合物在1.2上进行接枝聚合而制备的，
1.1 5-97wt％下列单体的混合物
1.1.1 5-50wt％丙烯腈、甲基丙烯腈、马来酸酐、N-取代马来酰亚胺或其混合物，和
1.1.2 95-50wt％苯乙烯、α-甲基苯乙烯、包含取代环的苯乙烯、甲基丙烯酸甲酯或其混合物，
1.2 95-3wt％至少一种玻璃化转变温度TG＜10℃的橡胶，和
2. 0-95wt％(当使用通过溶液、悬浮或本体聚合获得的接枝共聚物时)或20-95wt％(当使用通过乳液聚合获得的接枝共聚物时)至少一种热塑性树脂，其是通过溶液、悬浮或本体聚合由下列单体制备的：
2.1 5-50wt％丙烯腈、甲基丙烯腈、马来酸酐、N-取代马来酰亚胺或其混合物，和
2.2 95-50wt％苯乙烯、α-甲基苯乙烯、包含取代环的苯乙烯、甲基丙烯酸甲酯或其混合物。
3.根据权利要求1的复合材料，其中酚化合物B具有如下结构：
4.根据权利要求1的复合材料，其中酚化合物具有如下结构：
5.根据权利要求1的复合材料，其中另外的材料选自铝、钢、聚氯乙烯、聚对苯二甲酸乙二酯、聚对苯二甲酸丁二酯、聚碳酸酯、聚酰胺、聚乙烯和聚丙烯以及木材。
6.根据权利要求1的复合材料，其中ABS组分粘合到另外的材料上。
7.根据权利要求1的复合材料，其中ABS组分通过环氧树脂或丙烯酸酯粘合剂粘合到另外的材料上。
8.ABS组分在制备复合材料方面的应用，ABS组分包括：
A)ABS聚合物和
B)0.05-5wt％至少一种包含至少一个空间位阻羟基基团的酚，所述基团选自通式(I)-(IV)的结构单元：
其中R代表C10-C18烷基。
9.根据权利要求1-6的复合材料在制备模制品、片材和板条方面的应用。
10.由根据权利要求1-6的复合材料获得的模制品、片材和板条。
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| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| DE10127748A DE10127748A1 (de) | 2001-06-07 | 2001-06-07 | Verbund enthaltend ABS |
| DE10127748.2 | 2001-06-07 |
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| CN1541250A true CN1541250A (zh) | 2004-10-27 |
| CN100354366C CN100354366C (zh) | 2007-12-12 |
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| US (1) | US20030008948A1 (zh) |
| EP (1) | EP1399509A1 (zh) |
| JP (1) | JP2004527645A (zh) |
| KR (1) | KR20040010685A (zh) |
| CN (1) | CN100354366C (zh) |
| DE (1) | DE10127748A1 (zh) |
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| WO (1) | WO2002098978A1 (zh) |
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| US5883187A (en) * | 1995-05-16 | 1999-03-16 | Bayer Antwerpen S.A./N.V. | Polymer composition with improved toughness |
| US5698622A (en) * | 1996-03-14 | 1997-12-16 | Bayer Ag | Stabilisation of ABS graft polymers using dithiodipropionic acid |
| DE19715595A1 (de) * | 1997-04-15 | 1998-10-22 | Bayer Ag | Emulsionsfrei hergestellte ABS-Formmassen mit sehr hohrer Kerbschlagzähigkeit |
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2001
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- 2002-05-27 JP JP2003502092A patent/JP2004527645A/ja active Pending
- 2002-05-27 KR KR10-2003-7015949A patent/KR20040010685A/ko active IP Right Grant
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- 2002-05-27 MX MXPA03011241A patent/MXPA03011241A/es not_active Application Discontinuation
- 2002-05-27 EP EP02743108A patent/EP1399509A1/de not_active Withdrawn
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| Publication number | Publication date |
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| JP2004527645A (ja) | 2004-09-09 |
| CN100354366C (zh) | 2007-12-12 |
| KR20040010685A (ko) | 2004-01-31 |
| US20030008948A1 (en) | 2003-01-09 |
| MXPA03011241A (es) | 2004-03-18 |
| EP1399509A1 (de) | 2004-03-24 |
| DE10127748A1 (de) | 2002-12-12 |
| WO2002098978A1 (de) | 2002-12-12 |
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