CN113366048A - 导电模塑料 - Google Patents
导电模塑料 Download PDFInfo
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- CN113366048A CN113366048A CN201980084153.XA CN201980084153A CN113366048A CN 113366048 A CN113366048 A CN 113366048A CN 201980084153 A CN201980084153 A CN 201980084153A CN 113366048 A CN113366048 A CN 113366048A
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- weight
- molding compound
- filler
- molding
- polyether
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- 238000000465 moulding Methods 0.000 title claims abstract description 75
- 150000001875 compounds Chemical class 0.000 title claims abstract description 48
- 239000004952 Polyamide Substances 0.000 claims abstract description 99
- 229920002647 polyamide Polymers 0.000 claims abstract description 99
- 229920000570 polyether Polymers 0.000 claims abstract description 34
- 239000000945 filler Substances 0.000 claims abstract description 33
- 239000004721 Polyphenylene oxide Substances 0.000 claims abstract description 28
- 229920001519 homopolymer Polymers 0.000 claims abstract description 23
- 125000004427 diamine group Chemical group 0.000 claims abstract description 22
- 125000002887 hydroxy group Chemical group [H]O* 0.000 claims abstract description 15
- 239000000206 moulding compound Substances 0.000 claims abstract description 12
- 238000002844 melting Methods 0.000 claims abstract description 11
- 230000008018 melting Effects 0.000 claims abstract description 11
- 125000002924 primary amino group Chemical group [H]N([H])* 0.000 claims abstract description 10
- 238000004519 manufacturing process Methods 0.000 claims abstract description 8
- 229920006114 semi-crystalline semi-aromatic polyamide Polymers 0.000 claims abstract description 8
- 229920001577 copolymer Polymers 0.000 claims abstract description 7
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- 239000000203 mixture Substances 0.000 claims description 49
- 230000004888 barrier function Effects 0.000 claims description 21
- 125000004432 carbon atom Chemical group C* 0.000 claims description 17
- 239000004014 plasticizer Substances 0.000 claims description 11
- 238000000034 method Methods 0.000 claims description 8
- 239000012778 molding material Substances 0.000 claims description 7
- 239000000470 constituent Substances 0.000 claims description 6
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- 239000010410 layer Substances 0.000 description 82
- 239000000446 fuel Substances 0.000 description 38
- 238000012360 testing method Methods 0.000 description 38
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- UFRKOOWSQGXVKV-UHFFFAOYSA-N ethene;ethenol Chemical compound C=C.OC=C UFRKOOWSQGXVKV-UHFFFAOYSA-N 0.000 description 5
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- CJZGTCYPCWQAJB-UHFFFAOYSA-L calcium stearate Chemical class [Ca+2].CCCCCCCCCCCCCCCCCC([O-])=O.CCCCCCCCCCCCCCCCCC([O-])=O CJZGTCYPCWQAJB-UHFFFAOYSA-L 0.000 description 2
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- TVIDDXQYHWJXFK-UHFFFAOYSA-N dodecanedioic acid Chemical compound OC(=O)CCCCCCCCCCC(O)=O TVIDDXQYHWJXFK-UHFFFAOYSA-N 0.000 description 2
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- FTWUXYZHDFCGSV-UHFFFAOYSA-N n,n'-diphenyloxamide Chemical class C=1C=CC=CC=1NC(=O)C(=O)NC1=CC=CC=C1 FTWUXYZHDFCGSV-UHFFFAOYSA-N 0.000 description 2
- BDJRBEYXGGNYIS-UHFFFAOYSA-N nonanedioic acid Chemical compound OC(=O)CCCCCCCC(O)=O BDJRBEYXGGNYIS-UHFFFAOYSA-N 0.000 description 2
- RIKCMEDSBFQFAL-UHFFFAOYSA-N octyl 4-hydroxybenzoate Chemical compound CCCCCCCCOC(=O)C1=CC=C(O)C=C1 RIKCMEDSBFQFAL-UHFFFAOYSA-N 0.000 description 2
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- WLJVNTCWHIRURA-UHFFFAOYSA-N pimelic acid Chemical compound OC(=O)CCCCCC(O)=O WLJVNTCWHIRURA-UHFFFAOYSA-N 0.000 description 2
- 229920000909 polytetrahydrofuran Polymers 0.000 description 2
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- KIDHWZJUCRJVML-UHFFFAOYSA-N putrescine Chemical compound NCCCCN KIDHWZJUCRJVML-UHFFFAOYSA-N 0.000 description 2
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- CXMXRPHRNRROMY-UHFFFAOYSA-N sebacic acid Chemical compound OC(=O)CCCCCCCCC(O)=O CXMXRPHRNRROMY-UHFFFAOYSA-N 0.000 description 2
- 230000003068 static effect Effects 0.000 description 2
- TYFQFVWCELRYAO-UHFFFAOYSA-N suberic acid Chemical compound OC(=O)CCCCCCC(O)=O TYFQFVWCELRYAO-UHFFFAOYSA-N 0.000 description 2
- 239000000126 substance Substances 0.000 description 2
- YAXWOADCWUUUNX-UHFFFAOYSA-N 1,2,2,3-tetramethylpiperidine Chemical class CC1CCCN(C)C1(C)C YAXWOADCWUUUNX-UHFFFAOYSA-N 0.000 description 1
- RTBFRGCFXZNCOE-UHFFFAOYSA-N 1-methylsulfonylpiperidin-4-one Chemical compound CS(=O)(=O)N1CCC(=O)CC1 RTBFRGCFXZNCOE-UHFFFAOYSA-N 0.000 description 1
- GUOSQNAUYHMCRU-UHFFFAOYSA-N 11-Aminoundecanoic acid Chemical compound NCCCCCCCCCCC(O)=O GUOSQNAUYHMCRU-UHFFFAOYSA-N 0.000 description 1
- QFGCFKJIPBRJGM-UHFFFAOYSA-N 12-[(2-methylpropan-2-yl)oxy]-12-oxododecanoic acid Chemical compound CC(C)(C)OC(=O)CCCCCCCCCCC(O)=O QFGCFKJIPBRJGM-UHFFFAOYSA-N 0.000 description 1
- ACZGCWSMSTYWDQ-UHFFFAOYSA-N 3h-1-benzofuran-2-one Chemical class C1=CC=C2OC(=O)CC2=C1 ACZGCWSMSTYWDQ-UHFFFAOYSA-N 0.000 description 1
- UJAWGGOCYUPCPS-UHFFFAOYSA-N 4-(2-phenylpropan-2-yl)-n-[4-(2-phenylpropan-2-yl)phenyl]aniline Chemical compound C=1C=C(NC=2C=CC(=CC=2)C(C)(C)C=2C=CC=CC=2)C=CC=1C(C)(C)C1=CC=CC=C1 UJAWGGOCYUPCPS-UHFFFAOYSA-N 0.000 description 1
- FJKROLUGYXJWQN-UHFFFAOYSA-M 4-hydroxybenzoate Chemical compound OC1=CC=C(C([O-])=O)C=C1 FJKROLUGYXJWQN-UHFFFAOYSA-M 0.000 description 1
- 229940090248 4-hydroxybenzoic acid Drugs 0.000 description 1
- YUXBNNVWBUTOQZ-UHFFFAOYSA-N 4-phenyltriazine Chemical class C1=CC=CC=C1C1=CC=NN=N1 YUXBNNVWBUTOQZ-UHFFFAOYSA-N 0.000 description 1
- NIXOWILDQLNWCW-UHFFFAOYSA-M Acrylate Chemical compound [O-]C(=O)C=C NIXOWILDQLNWCW-UHFFFAOYSA-M 0.000 description 1
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- XMWRBQBLMFGWIX-UHFFFAOYSA-N C60 fullerene Chemical class C12=C3C(C4=C56)=C7C8=C5C5=C9C%10=C6C6=C4C1=C1C4=C6C6=C%10C%10=C9C9=C%11C5=C8C5=C8C7=C3C3=C7C2=C1C1=C2C4=C6C4=C%10C6=C9C9=C%11C5=C5C8=C3C3=C7C1=C1C2=C4C6=C2C9=C5C3=C12 XMWRBQBLMFGWIX-UHFFFAOYSA-N 0.000 description 1
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Abstract
本发明公开了一种模塑料,其含有至少50重量%的半结晶聚酰胺组分,并且所述模塑料含有赋予所述模塑料导电性的填料,其中所述模塑料不具有低于50℃的微晶熔点(Tm),所述聚酰胺组分含有组分A和B,A)PA X.Y或PA Z型的PA均聚物,其中X表示二胺残基(DA),Y表示二羧基残基(DC),Z表示α,ω‑氨基酸残基;B)PA X'.Y'型的PA共聚物,其中X'表示二胺残基(DA'),Y'表示二羧基残基(DC');其中一部分二胺残基(DA')被具有至少两个氨基末端或至少两个羟基末端的聚醚取代;其中聚醚在组分A和B的总和中的比例为0.5重量%‑15重量%,并且其中填料的比例为2.5重量%‑6重量%,基于聚酰胺组分和填料的总质量。本发明还涉及制备所述模塑料和使用所述模塑料的方法,以及包含所述模塑料的中空型材。
Description
本发明涉及作为模塑料(moulding compounds)的成分的半结晶聚酰胺组分,其中该聚酰胺组分不具有低于50℃的微晶熔点(Tm)。
用于机动车辆中液体或气体介质传送的柔性管是众所周知的。这个问题以前通过由聚酰胺或其他热塑性模塑料制成的单层管令人满意地解决。在这些单层管的情况下发现,即使在机动车辆的使用寿命内,安装后存在的机械性能(如高断裂伸长率和高耐冲性)也不会由于冷或热的影响或由于与介质接触而明显改变,以致于导致管道失效。
更严格的环境法规已经导致远离用作燃料管线的单层管和单层燃料容器的进一步开发和使用。在这两种情况下,汽车工业不仅需要足够的耐燃油性,而且要求对燃料组分有改进的阻隔效果,以减少其排放。这导致了使用阻隔层材料的多层中空体的发展。这种多层复合材料,其不仅包含阻隔层,而且还包含基于脂族聚酰胺的其他层,例如由EP 1216826A2已知。
由于聚酰胺具有良好的机械性能、低的吸水能力和对环境影响的不敏感性,因此聚酰胺是用于内层和外层的有用材料。相邻层之间的粘合是期望的,并且可以用插入的粘合促进层来确保。在汽车工业中,一段时间以来,发动机舱内的温度越来越高,因此要求在这些温度下使用的空心体的稳定性。包括基于例如聚烯烃的粘合促进层的技术方案由于其耐热变形性低而不合适。EP1216826A2通过使用粘合促进层解决了该问题,所述粘合促进层包含选自PA6、PA66和PA6/66的聚酰胺、任选存在的聚胺-聚酰胺共聚物,和选自PA11、PA12、PA612、PA1012和PA1212的聚酰胺。
例如,为了降低机动车辆发动机的能量消耗,在保持相同性能的同时减小部件尺寸的“缩小”的趋势不仅导致在发动机舱中占主导的温度的升高,而且导致喷射阀尺寸的减小。这些阀是将燃料喷射到内燃机的进气道或燃烧室中的喷嘴。燃料中存在的极性组分要求所用的多层管能抵抗从所用材料中提取成分。US 6467508描述了这样的提取物在燃料中沉淀和可能堵塞喷射阀的问题。该问题通过在内层中使用“低沉淀聚酰胺”来解决。“低沉淀聚酰胺”是洗涤过的聚酰胺,其通过不方便且昂贵的预先用甲醇萃取获得。以这种方式,除去麻烦的成分,例如低聚物。
随着喷嘴的尺寸逐渐减小,汽车工业也不仅要求减少在燃料中沉淀出来的提取物,而且还要求减少可溶于燃料中的提取物。由于引进混合动力车,增强了这一要求,因为这些车辆的内燃机不长时间使用。因此,燃料中的可溶性提取物也会通过干燥导致喷嘴堵塞。提取物不仅是US 6467508中描述的低聚物,而且是添加剂(例如所用模塑料的增塑剂和稳定剂)。
在DE 3 724 997 C2和DE 2 716 004 C3以及EP 0 566 755 B1中,以月桂内酰胺为单体的聚醚-嵌段-酰胺用于聚酰胺嵌段。与尼龙-12相应的改性混合物也在Polyamid-Kunststoffhandbuch[Plastics Handbook-Polyamide],3/4,1998,Carl Hanser Verlag,第872页,第8.3.3段中提及。这些共混物基于尼龙-12嵌段与均聚酰胺的共结晶显示出部分相容性。
EP1884356公开了聚酰胺/聚酰胺弹性体(TPE-A)的共混物;在可能的添加剂列表中也提及了导电添加剂的添加。所公开的共混物同时含有大量的聚醚酰胺和大量的基于聚烯烃的抗冲改性剂。
例如在EP0459862B1和CH642982中描述了聚醚酰胺的制备。这里聚醚酰胺由在两个链末端具有羧基的聚酰胺序列与在两个链末端具有氨基的聚氧化烯序列制备。
WO 2017/121961 A1和WO 2017/121962 A1要求保护多层管,其中内层具有至少三种具有不同链长的不同聚酰胺。这些层也可以包括聚醚-嵌段-酰胺;它们也可以是导电的。
典型的热塑性塑料具有1016-1014欧姆(Ω)范围内的比表面电阻,因此可以建立高达15 000伏的电压。有效的抗静电剂可以将塑料的比表面电阻降低到1010-109欧姆。相反,如果将塑料用于大型装置的电子元件中,例如用于变压器或电气开关设备制造领域,或用于汽车和飞机结构的多种应用中,则必须达到高得多的静电荷耗散水平。在此必须使用导电的模塑料,其必须具有小于109欧姆的比表面电阻。另外关键的是,在这种塑料应用中,不仅表面电阻,而且通过具有至多几毫米厚度的塑料部件的体积电阻必须在非常相同的范围内,并且在通过注塑生产的部件的情况下,通常难以防止各向异性效应的发展。
因此,对于导电塑料部件的制造,仅可以使用已经导电的塑料,例如尤其是聚苯胺,或者通过使用炭黑,尤其是导电炭黑、碳纤维、石墨、石墨烯和/或碳纳米管(CNT),使上述可表征为电绝缘体的塑料导电。
碳纳米管,连同石墨、金刚石、无定形碳和富勒烯,是元素碳的另一种多晶型物。碳原子在此以六边形排列。该结构对应于卷起的石墨的单原子或多原子层,以便形成直径通常为几纳米且长度高达几毫米的中空圆柱体。多壁和单壁碳纳米管之间的基本区别通常在文献中也缩写为MWNT和SWNT。由于范德华力,碳纳米管具有强烈的结合成束的倾向,因此在挤出过程中通过强剪切力在没有显著缩短的情况下解缠结/分散是必要的。典型的商业产品可从各制造商获得,在此通过实例提及以下产品:Bayer、Cyclics(以前称为Electrovac)、Nancycol和Arkema及其C150P(德国Bayer AG的商标)、BaytubesC 150HP、Baytubes C 70P、Electrovac HTF 110FF、NC 7000(比利时NanocylSA的商标)和Graphistrength C100品级。其他制造商以母料形式提供CMT,例如Hyperion和C-聚合物。
因此,本发明所解决的问题是提供导电模塑料,其不需要任何低分子量增塑剂或其他可提取物来改善机械性能和改善抗老化性。
该问题通过作为模塑料的成分的半结晶聚酰胺组分来解决,其中该聚酰胺组分不具有低于50℃的微晶熔点(Tm),如在下文和权利要求中详细描述的。
本发明提供一种模塑料,其包含至少50重量%、优选60重量%、更优选70重量%、特别优选80重量%、尤其优选至少90重量%的半结晶聚酰胺组分,并且包含赋予模塑料导电性的填料,其特征在于所述模塑料不具有低于50℃的微晶熔点,
其中所述聚酰胺组分包含组分A和B,
A PA X.Y或PA Z型的PA均聚物,其中X表示二胺残基(DA),Y表示二羧基残基(DC),Z表示α,ω-氨基酸残基;
B PA X'.Y'的PA共聚物,其中X'表示二胺残基(DA'),Y'表示二羧基残基(DC');
其中一些二胺残基(DA')被具有至少两个氨基末端或至少两个羟基末端的聚醚取代;
其中聚醚在组分A和B的总和中的比例为0.5重量%-15重量%,
且其中填料的比例为2.5重量%-6重量%,基于聚酰胺组分和填料的总质量,
其中至多10mol%的PA均聚物可以由其他酰胺形成单元形成,
其中至多10mol%的二胺残基(DA')可以被仅具有一个氨基末端或仅具有一个羟基末端的聚醚取代。
本发明还提供了根据本发明所述的模塑料用于制备中空型材的用途。
本发明还提供了单层或多层中空型材,其具有至少一个由根据本发明所述的模塑料组成的层。
下文通过实施例描述了本发明所述的模塑料和包含本发明所述的模塑料的成型体(例如中空型材)以及本发明的用途,但本发明并不限于这些示例性实施方案。当下面提到化合物的范围、通式或类别时,这些不仅包括明确提及的化合物的相应范围或组,而且包括可通过提取单个值(范围)或化合物获得的化合物的所有子范围和子组。其中,在本说明书的上下文中引用文献的情况下,其全部内容旨在作为本发明公开内容的一部分。其中,除非另有说明,否则在下文中给出的百分比数字是重量百分比。在组合物的情况下,除非另有说明,百分比数字是基于整个组合物。其中,除非另有说明,否则在下文中给出的平均值是质量平均值(重量平均值)。其中,除非另有说明,否则下文给出的测量值是在101 325Pa的压力和25℃的温度下测定的。
保护范围包括商业上惯用的根据本发明产品的成品和包装形式,包括其本身和任何缩小尺寸形式,其程度不在权利要求中限定。
聚醚的不同单元呈统计分布。统计分布是具有任何期望数量的嵌段和任何期望序列的嵌段构造,或者它们具有随机分布;它们还可以具有交替结构或者在聚合物链上形成梯度;更特别地,它们也可形成任何混合形式,其中具有不同分布的基团可任选地彼此跟随。作为实施方案的结果,特定实施方案可能导致对统计分布的限制。对于所有不受限制影响的区域,统计分布没有变化。
根据本发明所述的模塑料的一个优点是具有由本发明所述的模塑料组成的内层的单层或多层中空体具有高的抗冲蚀性(washout resistance)。这通过根据ASTM D471-15"Reference Fuel I"使用测试燃料在实施例中所述的管上测试来显示。测试燃料的特征是其含有15体积%的甲醇。测定抗冲蚀性的其他方法可为本领域已知的;在实施例中详述了根据本发明优选的方法。在此可以提取可溶性组分以及不溶性组分。优选地,每平方米测试试样的内表面小于6g的可溶性组分从测试试样中提取,优选地小于5.5g/m2。
本发明的模塑料的另一优点是由组分A、B和C组成的聚酰胺组分的结晶度低于以相同量包括相同组分A和C的混合物的结晶度。
具有由本发明的模塑料形成的内层和具有阻隔层的本发明的多层中空体的优点是低燃料渗透性。这通过根据ASTM D471-15“Reference Fuel I”使用测试燃料在实施例中所述的管上测试来显示。测试燃料的特征是其含有15体积%的甲醇。测定抗冲蚀性的其他方法可为本领域已知的;在实施例中详述了根据本发明优选的方法。
在一天的测试持续时间内,在60℃下储存时,优选有不超过6g/m2从测试试样扩散出,优选小于5.5g/m2,更优选小于5.0g/m2,尤其优选小于4.5g/m2。
酰胺形成单元是α,ω-氨基酸残基或二胺残基与二羧基残基的组合。优选的α,ω-氨基酸残基是游离氨基酸或其内酰胺,更优选ε-己内酰胺、11-氨基十一酸、12-氨基月桂酸或相应的月桂内酰胺。
二胺残基是具有在每个末端带有氨基的烃的残基,其中氨基可以形成聚合物的末端,但通常有助于具有化合价的链形成。
优选的烃是脂族烃,更优选具有2-18个碳原子,特别优选3-14个碳原子,尤其优选4-12个碳原子。如果烃具有多于3个碳原子,则这些是直链、支链或环状的,优选直链,更优选至多6个碳原子的直链。
特别优选的二胺残基是乙二胺、1,4-二氨基丁烷、1,6-二氨基己烷、1,10-二氨基癸烷、1,12-二氨基十二烷;特别优选1,6-二氨基己烷。
二羧基残基(DC)是具有在每个末端带羧基的烃的残基,其中羧基可以形成聚合物的末端,但通常有助于作为具有化合价的羰基的链形成。
优选的烃是脂族烃,更优选具有3-18个碳原子,特别优选具有6-14个碳原子,尤其优选具有8-12个碳原子。所述烃进一步优选是直链、支链或环状的,更优选是直链的。
优选的二羧基残基是琥珀酸、戊二酸、己二酸、庚二酸、辛二酸、壬二酸、癸二酸、十二烷二酸的残基,特别优选十二烷二酸的残基。
所述PA均聚物包括用于组分A的聚酰胺(PA);优选的聚酰胺是PA 6、PA 11、PA 12、PA 4.6、PA 6.6、PA 6.9、PA 6.10、PA6.12、PA9.10、PA9.12、PA10.10、PA10.12、PA12.12;更优选PA 6.6、PA 6.10、PA6.12、PA10.10;特别优选PA 6.10、PA 6.12、PA 10.10,尤其优选PA6.12。
基于PA共聚物的总质量,组分B的PA共聚物的聚醚含量优选为8重量%-30重量%,更优选9重量%-25重量%,特别优选10重量%-20重量%,尤其优选12重量%-18重量%。
所述聚醚优选具有3至50个重复单元,更优选4至40个,特别优选5至30个,尤其优选6至20个,其中重复单元通过氧原子彼此连接。
聚醚优选不含不具有任何氢原子的氮原子,并且进一步优选在聚合物链中不含式-NH-、=NH的氨基。
更优选地,所述聚醚仅具有亚烷基氧基单元;优选地,如果存在具有3-18个碳原子的亚烷基氧基单元,则聚合物具有立构规整度,即全同立构、间同立构、杂同立构、半全同立构、无规立构。
特别优选的聚醚由亚乙基氧基、亚丙基氧基和亚丁基氧基单元或其混合物组成,其中混合物是随机的。尤其优选的聚醚由亚乙基氧基和亚丙基氧基单元组成,或由正亚丁基氧基单元组成,或由亚丙基氧基单元组成。
所述聚醚优选具有数均分子量Mn不超过5000g/mol,特别优选不超过2000g/mol,尤其优选不超过1000g/mol,其中下限至少为200g/mol,优选300g/mol,更优选400g/mol。
所述聚醚优选不具有多于两个氨基末端或两个羟基末端,更优选具有恰好两个氨基末端或两个羟基末端。
基于组分A和B的总质量,本发明的模塑料的聚酰胺组分优选具有1重量%-12重量%,优选1.5重量%-9重量%,特别优选2.0重量%-8重量%,尤其优选2.5重量%-7重量%的聚醚含量。
对于酰胺形成单元中的碳原子数,所述聚酰胺组分的PA共聚物和PA均聚物的链长优选彼此相差平均不超过10%,其中所述差基于所述链长的较高值。在使用PA共聚物PA10.12和PA均聚物如PA10.10的情况下,PA10.12的平均值为11,因此差值为9.1%。
本发明的模塑料中,基于聚酰胺组分和用于提高导电性的填料的总质量,即组分A、B和C的总质量,用于提高导电性的填料(组分C)的比例为2.5重量%-6重量%。2.5重量%的下限具有导电性足够高和电阻足够低的优点,以便能够用于大型设备的电子元件和汽车和飞机结构中。填料浓度大于6重量%进一步导致小的缺口抗冲击性,这表明在过高的填料浓度下材料的脆化。
用于增加导电性的优选填料不形成聚集体;因此,在引入剪切力时它们是可分散的。
进一步优选地,根据本发明的模塑料的结晶度低于包括等量的相同组分A和C(用于增加导电性的填料)的混合物的结晶度,其中模塑料的任何其他成分在种类和量上同样相同。
结晶度由现有技术方法确定;结晶度优选通过等式(1)计算
本发明范围内的参数Tm、Tg和ΔHm是借助DSC测定的,优选根据EN ISO 11354-1:2016D测定,更优选如实施例中所述。
用于计算结晶度XC的值ΔHm 0取自表格,例如van Krevelen“Properties ofPolymers”,第4版,2009年。优选地假设以下值:
本发明的模塑料优选不添加任何离子液体以提高导电性,例如在EP2635638A1(US20130299750A1)中所述。进一步优选地,根据本发明的模塑料不包括任何元素形式的金属。
优选地,根据本发明的模塑料不含增塑剂,优选不含低分子量增塑剂。本文中的增塑剂列于DIN EN ISO 1043-3:2017中,以及例如在醇组分中具有2-20个碳原子的对羟基苯甲酸的酯或在胺组分中具有2-12个碳原子的芳基磺酸的酰胺,优选苯磺酸的酰胺;对羟基苯甲酸乙酯、对羟基苯甲酸辛酯、对羟基苯甲酸异十六烷基酯、N-正辛基甲苯磺酰胺、N-正丁基苯磺酰胺或N-2-乙基己基苯磺酰胺。
本发明的模塑料优选通过在捏合单元中熔融混合,即采用剪切力由各组分制备。
因此,本发明还提供了一种制备本发明的模塑料的方法,其中各组分通过熔融混合进行混合。
本发明的模塑料的各组分可以同时或依次加入。尽管在优选的实施方案中,在母料制备的情况下,填料可以首先分散在组分A或B中(尤其是在组分B中),在这种情况下,随后用母料中不存在的相应组分B或A稀释所制备的母料,但非常特别优选其中通过熔融混合同时混合各成分A和B以及填料的制备本发明的模塑料的方法。本发明的模塑料的任何其他成分可与组分A和B以及填料同时加入或在其后加入。
优选的碳纳米管通常采用由石墨层形成的管的形式。石墨薄层(lamina)以同心方式围绕圆柱体轴线布置。碳纳米管也称为碳纳米纤丝。它们的长径比至少为5,优选至少为100,更优选至少为1000。纳米纤丝的直径通常在0.003-0.5μm的范围内,优选在0.005-0.08μm的范围内,更优选在0.006-0.05μm的范围内。碳纳米纤丝的长度通常为0.5-1000μm,优选0.8-100μm,更优选1-10μm。碳纳米纤丝具有中空的、圆柱形的核。该空腔的直径通常为0.001-0.1μm,优选地为0.008-0.015μm。在碳纳米管的典型实施方案中,空腔周围的纤丝的壁由例如8个石墨薄层组成。碳纳米纤丝在此可以采取直径高达1000μm的附聚物形式,其由多个纳米纤丝组成。附聚物可具有鸟巢、精梳纱或开放网眼结构的形式。碳纳米管例如在含有含碳气体和金属催化剂的反应器中合成,如US5643502A中所述。
除了多壁碳纳米管(MWCNT)之外,根据本发明也可以使用单壁碳纳米管(SWCNT)。SWCNT通常具有几纳米范围内的直径,但是相对于它们的横截面,其长度相当大,通常为几微米的范围。SWCNT的结构衍生自单原子石墨薄层(石墨烯),其可以想象为卷起以形成无缝圆柱体。SWCNT可以是优异的电导体。可获得的电流密度109A/cm2比铜或银的金属线的情况高约1000倍。SWCNT的生产描述于例如US5424054中。
进一步优选的是包含至少70重量%,特别优选80重量%,尤其优选至少90重量%的半结晶聚酰胺组分并且包含赋予模塑料导电性的填料的模塑料,其特征在于所述模塑料不具有低于50℃的微晶熔点,
其中所述聚酰胺组分包含组分A和B,
A PA X.Y或PA Z型的PA均聚物,其中X表示二胺残基(DA),Y表示二羧基残基(DC),Z表示α,ω-氨基酸残基;
B PA X'.Y'型的PA共聚物,其中X'表示二胺残基(DA'),Y'表示二羧基残基(DC');
其中一些二胺残基(DA')被具有两个氨基末端或两个羟基末端的聚醚取代;
其中聚醚在组分A和B的总和中的比例为0.5重量%-15重量%,
并且其中填料的比例为2.5重量%-6重量%,基于聚酰胺组分和填料的总质量;
其中至多10mol%的PA均聚物可以由其他酰胺形成单元形成;
其中组分B的PA共聚物具有8重量%-30重量%的聚醚含量,基于PA共聚物的总质量。
进一步优选的是包含至少70重量%,特别优选80重量%,尤其优选至少90重量%的半结晶聚酰胺组分并且包含赋予模塑料导电性的填料的模塑料,其特征在于所述模塑料不具有低于50℃的微晶熔点,
其中所述聚酰胺组分包含组分A和B,
A PA X.Y或PA Z型的PA均聚物,其中X表示二胺残基(DA),Y表示二羧基残基(DC),Z表示α,ω-氨基酸残基;
B PA X'.Y'型的PA共聚物,其中X'表示二胺残基(DA'),Y'表示二羧基残基(DC');
其中一些二胺残基(DA')被具有两个氨基末端或两个羟基末端的聚醚取代;
其中聚醚在组分A和B的总和中的比例为0.5重量%-15重量%,
并且其中填料的比例为2.5重量%-6重量%,基于聚酰胺组分和填料的总质量;
其中至多10mol%的PA均聚物可以由其他酰胺形成单元形成;
其中所述聚醚具有不超过5000g/mol的数均分子量Mn;
其中对于酰胺形成单元中的碳原子数,所述聚酰胺组分的PA共聚物的链长和PA均聚物的链长彼此相差平均不超过10%,其中所述差基于所述链长的较高值。
进一步优选的是包含至少70重量%,特别优选80重量%,尤其优选至少90重量%的半结晶聚酰胺组分并且包含赋予模塑料导电性的填料的模塑料,其特征在于所述模塑料不具有低于50℃的微晶熔点,
其中所述聚酰胺组分包含组分A和B,
A PA均聚物选自PA 6、PA 11、PA 12、PA 4.6、PA 6.6、PA 6.9、PA6.10、PA 6.12、PA9.10、PA 9.12、PA 10.10、PA 10.12、PA12.12;
B PA X'.Y'型的PA共聚物,其中X'表示二胺残基(DA'),Y'表示二羧基残基(DC');
其中一些二胺残基(DA')被具有两个氨基末端或两个羟基末端的聚醚取代;
其中聚醚在组分A和B的总和中的比例为0.5重量%-15重量%,
并且其中填料的比例为2.5重量%-6重量%,基于聚酰胺组分和填料的总质量;
其中至多10mol%的PA均聚物可以由其他酰胺形成单元形成;
其中模塑料的结晶度低于包括等量的相同组分A和用于增加导电性的填料的混合物的结晶度,其中模塑料的任何其他成分在种类和量上同样相同。
本发明的模塑料优选含有其他添加剂。
优选的添加剂是氧化稳定剂、UV稳定剂、水解稳定剂、抗冲改性剂、颜料、染料和/或加工助剂。
在优选的实施方案中,模塑料包含有效量的氧化稳定剂,更优选包含有效量的氧化稳定剂与有效量的含铜稳定剂的组合。合适的氧化稳定剂的实例包括芳族胺、空间位阻酚、亚磷酸盐(phosphites)、亚膦酸酯(phosphonites)、硫代增效剂(thiosynergists)、羟胺、苯并呋喃酮衍生物、丙烯酰基改性的酚等。许多类型的这种氧化稳定剂是可商购的,例如商品名为Naugard 445、Irganox 1010、Irganox 1098、Irgafos 168、P-EPQ或LowinoxDSTDP。通常,所述模塑料含有约0.01重量%-约2重量%,优选约0.1重量%-约1.5重量%的氧化稳定剂。
此外,所述模塑料还可以包含HALS型的UV稳定剂或光稳定剂。合适的UV稳定剂主要是有机UV吸收剂,例如二苯甲酮衍生物、苯并三唑衍生物、草酰苯胺(oxalanilides)或苯基三嗪。HALS型光稳定剂是四甲基哌啶衍生物;这些是作为自由基清除剂的抑制剂。UV稳定剂和光稳定剂可以有利地组合使用。两者中有许多类型是市售的;关于剂量,可以遵循制造商的说明。
所述模塑料可另外包含水解稳定剂,例如单体、低聚或聚合的碳二亚胺或双噁唑啉。
所述模塑料可进一步包含抗冲改性剂。用于聚酰胺模塑料的抗冲改性橡胶构成了现有技术的一部分。它们含有源自不饱和官能化合物的官能团,所述不饱和官能化合物包含在主链聚合物中或接枝到主链上。最常用的是用马来酸酐自由基接枝的EPM或EPDM橡胶。这种橡胶也可与未官能化的聚烯烃,例如全同立构聚丙烯一起使用,如EP0683210A2(US5874176A)中所述。
合适的颜料和/或染料的实例包括铁氧化物、锌硫化物、群青、苯胺黑、珠光颜料。
合适的加工助剂的实例包括石蜡、脂肪醇、脂肪酸酰胺、硬脂酸盐如硬脂酸钙、石蜡、褐煤酸酯或聚硅氧烷。
本发明的多层中空型材具有至少一个由本发明的模塑料制成的层,该层与液体直接接触。这优选地是中空体的最内层。
所述液体优选是包含烃和至少一种醇的化学物质的混合物;所述液体更优选地是适合作为内燃机的动力燃料的燃料;所述燃料特别优选是机动车辆燃料,例如柴油或汽油。
所述燃料优选包含具有1至8个碳原子的醇,更优选甲醇、乙醇、丙醇、丁醇或戊醇。具有至少三个碳原子的醇可以是它们的n形式,即直链的和具有末端羟基的,或它们的各种异构形式;这里的羟基可以是伯、仲或叔羟基,优选伯羟基。更优选地,至少80体积%的醇是具有末端羟基的直链烃。
所述燃料优选包括至少7体积%,更优选至少10体积%,特别优选至少13体积%,尤其优选至少16体积%的醇。
根据本发明的单层或多层中空体优选是管或容器,优选是燃料传导系统的组件,优选是燃料管线或燃料箱。
由本发明的模塑料制备的优选与液体接触的层是导电的。中空体具有不大于109Ω/平方的比表面电阻率,优选不大于106Ω/平方。合适的测试方法是现有技术中已知的;优先考虑如2004年11月的SAE J 2260中所述测定比表面电阻率。
根据本发明的优选的多层中空体具有所谓的阻隔层。该阻隔层对于燃料组分具有非常低的扩散系数。用于阻隔层的合适材料是氢氟烃和乙烯醇聚合物。优选的多层中空体优选具有所谓的EVOH阻隔层。EVOH是乙烯和乙烯醇的共聚物。共聚物中的乙烯含量优选为20-45mol%,尤其是25-35mol%。许多等级的商品是可商购的。通过举例的方式参考来自Kuraray EVAL Europe的公司手册“Introduction to Kuraray EVALTM Resins”,版本1.2/9810。除了根据现有技术的EVOH之外,阻隔层可以含有通常用于阻隔层应用的其他添加剂。这种添加剂通常是EVOH供应商的技术诀窍的一部分。
根据本发明的优选的多层中空体具有阻隔层(SpS)和作为最内层(Si)的由根据本发明的模塑料制备的层,其中中空体具有根据2004年11月的SAE J 2260不大于106Ω/平方的比表面电阻率。
在优选的多层中空体的阻隔层(SpS)和最内层(Si)之间可以设置另外的层,优选地至少一个层(HVi),其确保Si和SpS之间的粘合。优选地,在SpS和Si之间仅设置粘合促进层。如果SpS和Si之间的粘合性足够大,当然可以省去粘合促进层(HVi)。
阻隔层和根据本发明的模塑料层之间的粘合促进剂是本领域技术人员已知的;优选的粘合促进剂基于聚酰胺,优选由PA6.12和PA 6的混合物组成,更优选由抗冲改性的聚酰胺组成,特别优选包含60重量%-80重量%的PA 6.12、10重量%-25重量%的PA 6和5重量%-15重量%的抗冲改性剂,其中选择质量比以使其加起来为100重量%。
优选地,设置在根据本发明的优选的中空体中的阻隔层的内侧上的层不含如上所定义的增塑剂。进一步优选地,这些层仅包括所需的确切量的添加剂,例如稳定剂和加工助剂。
根据本发明的优选中空体优选地在阻隔层的外侧上具有至少一个另外的层。这些外层同样优选是包含至少50重量%、更优选至少60重量%、甚至更优选至少70重量%、特别优选至少80重量%、尤其优选至少90重量%聚酰胺的层。
这些聚酰胺优选是如上所述的PA X.Y或PA Z型的PA均聚物。优选的中空体的外层(Sa)的PA均聚物与最内层(Si)的PA均聚物不相同。优选地,外层的PA均聚物(Sa)是PA Z型的PA,更优选PA11或PA12,特别优选PA12。
在根据本发明的优选中空体的外层(Sa)和阻隔层(SpS)之间可以设置另外的层,优选地为确保Sa和SpS之间的粘合的至少一个层(HVa)。优选地,在Sa和SpS之间仅设置粘合促进层。如果Sa和SpS之间的粘合性足够大,当然可以省去粘合促进层(HVa)。
所述粘合促进层(HVa)优选地不含如上文所定义的增塑剂。进一步优选地,该层仅包括所需的确切量的添加剂,例如稳定剂和加工助剂。
优选地,粘合促进层HVi和HVa在它们的化学组成方面是相同的。
进一步优选的是多层中空型材,其具有至少一个由根据本发明的模塑料组成的层,其中该层与液体直接接触,并且另外具有至少一个阻隔层。
进一步优选的是多层中空型材,其具有至少一个由根据本发明的模塑料组成的层,并且另外具有至少一个氢氟烃或乙烯醇聚合物的阻隔层;其中设置在中空体中的阻隔层的内侧上的层不含增塑剂。
根据本发明的中空型材还可以被附加的弹性体层包覆。交联橡胶组合物和热塑性弹性体都适用于护套(sheathing)。可以在使用或不使用另外的粘合促进剂的情况下,例如通过共挤出、通过十字头模具挤出或通过在已挤出的多层管上滑动预制的弹性体软管,将护套施加到多层复合材料上。护套的厚度通常为0.1至4mm,优选为0.2至3mm。
合适的弹性体的实例包括氯丁橡胶、乙丙橡胶(EPM)、三元乙丙橡胶(EPDM)、表氯醇橡胶(ECO)、氯化聚乙烯、丙烯酸酯橡胶、氯磺化聚乙烯、硅橡胶、增塑PVC、聚醚酯酰胺或聚醚酰胺。
多层复合材料可以在一个或多个阶段中制造,例如通过单阶段方法,通过夹层模塑、共挤出、共挤出吹塑(例如包括3D吹塑、将型坯挤出到开放的半模中、3D型坯操作、抽吸吹塑、3D抽吸吹塑、顺序吹塑)或通过例如US5554425中所述的多阶段方法。
在下面的实验中将通过实施例阐明本发明。
在实施例中,使用以下组分/模塑料:
PA均聚物1:基于来自EVONIK Resource Efficiency GmbH的PA6.12(VESTAMIDD22)的挤出模塑料
PA均聚物2:基于来自EVONIK Resource Efficiency GmbH的PA10.10(VESTMIDDS22)的挤出模塑料
PA均聚物3:基于来自EVONIK Resource Efficiency GmbH的PA12(VESTAMIDL1901)的挤出模塑料
PEBA 1:基于来自EVONIK Resource Efficiency GmbH的PA6.12的挤出模塑料,其含有25重量%的摩尔质量为400g/mol的双氨基封端的聚醚(Elastamin RP-405,Huntsman)
PEBA 2:基于EVONIK Resource Efficiency GmbH的PA 10.10的挤出模塑料,其含有35.4重量%的具有650g/mol的摩尔质量的双羟基封端的聚醚(聚四氢呋喃)
PEBA 3:基于来自EVONIK Resource Efficiency GmbH的PA 12的挤出模塑料,其含有29重量%的具有1000g/mol摩尔质量的双羟基封端的聚醚(聚四氢呋喃)
EVAL:来自Kuraray的含有27mol%乙烯的EVOH(EVAL LA170B)
IM:抗冲改性剂:Exxelor VA1803(9%)+1%Lotader AX8900
稳定剂:Irgafos和Irganox的混合物
粘合促进剂:基于EVONIK Resource Efficiency GmbH的PA6.12(VESTAMIDSX8002或VESTAMID SX8080;SX8080具有与SX8002相同的指数,但不含增塑剂)的挤出模塑料
实施例1,模塑料:
在Haake捏合机(HAAKE Rheomix 600OS)中通过将各组分在熔体中混合而配混以下模塑料。
表1:
实施例1的模塑料的组成。
PEBA表示PA共聚物,PE表示聚醚,CNT表示碳纳米管;
PE的含量是指在模塑料中聚醚的重量比例,不考虑CNT的质量;
CNT的含量是基于总模塑料的质量比
模塑料13、23和33是根据本发明的模塑料。
实施例2,热性能的测定:
根据ISO 11357(Perkin-Elmer),通过DSC以20K/min的速率测定第1次加热过程中的玻璃化转变温度Tg和微晶熔点Tm,并由第2次加热过程中的熔融焓的测定计算结晶度XC。
表2:根据实施例2测定热性能;nd表示未测定的值
在所有情况下观察到,结晶度XC随着碳纳米管加入到基础聚合物中而升高。此外,在所有情况下都观察到当小部分基础聚合物被PEBA代替时,结晶度XC可以降低。本发明的模塑料不具有低于50℃的微晶熔点;这对于具有较低聚醚含量的模塑料34也是如此。
实施例3,中空型材的制造:
通过在来自Bellaform的多层管系统上共挤出,制备外径为8mm且总壁厚为1mm的五层管。
比较例仅内层(层I)的组成不同。
表3:实施例3的中空型材的层结构
实施例4:试验:
对来自实施例3的管进行以下试验:
a)拉伸试验(使用MLT):根据DIN EN ISO 527-1在100mm/min的引出速度下测试单层和多层管。测试试样具有约200mm的长度,夹紧长度为100mm,应变传感器间距为50mm。
b)冲击试验:根据DIN 73378在23℃下测量单层和多层管的抗冲击性。
用质量为880g的落锤,根据VWTL52435,在-25℃下测量单层和多层管的抗冲击性能。
用质量为500g的落锤,根据SAE J2260,在-40℃下测量单层和多层管的抗冲击性能。
对于所有测试,分析10个长度为约100mm的试样。应力测试之后目视检查是否有损坏。
c)分离试验:分离试验用Zwick BZ 2.5/TN1S拉伸试验机进行,拉伸装置和由金属制成的旋转偏转辊连接到该拉伸试验机上,以便能够将测试试样的各层彼此分离。使用根据DIN EN ISO 2411的分离试验,通过测量将两层彼此分离所需的力来测定两层之间的粘合性。为此,使用切割装置将长度为20cm的多层管的管段纵向分成三个部分。
在开始测量之前,使用卡尺在不同的点重复测量样品的宽度,取平均值进行评价。然后将一层的最初分离的末端保持在夹具中,该夹具以90°的角度连续地从第二层拉出所述层。
以50mm/min的测试速度将层拉开,同时记录所需的力(以牛顿为单位)对位移(以毫米为单位)的图。该图用于在平台区域(plateau region)中基于粘附接触区域的宽度确定以N/mm为单位的分离电阻。
d)燃料透过性:使用渗透测量测定在60℃静态储存的情况下,每天每米的管或每平方米的内管面积多少燃料渗透穿过燃料管线。为此目的,将在各情况下长度为300mm的管段在一端拧到压力密封的储存容器上并且称重,然后填充300ml的CM 15,并且关闭第二端。将这些测试试样储存在60℃强制通风的防爆加热箱中,再次称重填充的管,以便能够确定质量损失,并因此确定在特定时间间隔的燃料的渗透质量。有效渗透长度为285mm。
e)抗冲蚀性:通过测定冲蚀,确定在暴露于燃料之后,有多少g/m2内管表面以可溶和不溶成分的形式从多层复合材料中提取出来。为此目的,用CM15测试燃料完全填充长度为2m的管段并且关闭,并且在60℃下储存96h。冷却后,将管排空到烧杯中并用20ml的CM 15冲洗。将所得液体在23℃下储存24小时。然后将测试液体在23℃下减压过滤,用20ml的CM15冲洗。将过滤的介质在通风橱中在室温下蒸发。通过称重得到可溶性提取物。将过滤器在40℃下干燥24小时并称重。使用与过滤器原始重量的差来测定不溶性提取物。
如果少于6g/m2的可溶性成分和少于0.5g/m2的不溶性成分被冲蚀,则认为测试合格。
f)MLT的热老化性能描述(热风循环柜,在150℃下200h和在170℃下1h)
在热风循环柜中,将长度为约100或200mm的对应的单层管或多层管的管件在升高的温度下储存限定的时间段。在此应确保管件自由地悬挂在空气循环炉中而不彼此接触或不与金属表面接触。
管件的长度取决于随后的机械测试。如b)中所述,将长度为约100mm的测试试样用于管冲击测试。在150℃下储存200小时,随后在23℃/50%的相对湿度的标准气候条件下调节>24小时,如b)中所述进行管冲击试验。类似地对已经在170℃下预先储存1h的管件进行管冲击测试。
g)通过在60℃下用CM 15、CE10和FAM B进行燃料储存来测定绝缘电阻及其变化。
根据SAEJ 2260-1996对长度为42cm的至少三个管段测定电阻。为此,使内管表面在管端与具有限定长度和直径的塞子接触。使用10V与500V之间的测试电压来测量102至1014Ω范围内的电阻,并且使用塞子之间的内部管道面积将其转换为所需的具有单位“欧姆/平方”的表面电阻率。
然后,将管段的一端用螺丝拧到储存容器上并称重,然后装入300ml试验燃料(CM15),并将第二端封闭。管在储存容器下方,使得在储存和电测量期间,内管表面完全充满燃料。内层通过金属螺纹连接件与管端的支承套筒接触,并且在填充后直接测定电阻。将测试试样储存在60℃下强制通风的防爆加热箱中,并以固定的时间间隔冷却至23℃,测定电阻变化,测试时间为约1000小时。与电阻并行地,自由管横截面的绝对长度用螺纹连接件之间的卷尺确定,并且长度的变化用0%至5%范围内的千分表确定。
如果测定电阻小于106欧姆/面积,则认为测试合格。
试验燃料CE 10和CM 15和FAM B的组成在SAE J2260-1996的参考文献中;CM 15对应于ASTM D471-15,“Reference Fuel I”(异辛烷/甲苯,甲醇);FAM B对应于DIN 51604-2(1984)的测试液体;CE 10对应于根据ASTM D471-15的“燃料C”加上10±1体积%的乙醇的混合物。
结果示于表4。
表4:根据实施例3的管的试验结果
实施例5-具有不同填料含量的模塑料
首先,用Nanocyl双螺杆挤出机制备含填料的母料,基于具有10%CNT浓度的聚醚改性的聚酰胺(PA612.6T,研磨粉末)。
然后在双螺杆挤出机中稀释母料,加入聚酰胺、抗冲改性剂、稳定剂和染料。这样制得的模塑混合物的组分和填料含量如表5所示。
表5-配方
使用模塑料制备测试试样。对于缺口冲击试验,这些是尺寸为170×10×4mm3的注塑/多用途测试试样。对于电气测试,挤出厚度为1mm的带。
下表6示出了缺口冲击试验和电气试验的结果以及试验条件。
表6-试验
明显看出缺口抗冲击性降低6%以上。另外,比电阻低于2.5%过高。
Claims (12)
1.模塑料,其包含至少50重量%的半结晶聚酰胺组分,并且包含赋予所述模塑料导电性的填料,
其特征在于,所述模塑料不具有低于50℃的微晶熔点(Tm),
其中所述聚酰胺组分包含组分A和B,
A PA X.Y或PA Z型的PA均聚物,其中X表示二胺残基(DA),Y表示二羧基残基(DC),Z表示α,ω-氨基酸残基;
B PA X'.Y'型的PA共聚物,其中X'表示二胺残基(DA'),Y'表示二羧基残基(DC');
其中一些二胺残基(DA')被具有至少两个氨基末端或至少两个羟基末端的聚醚取代;
其中聚醚在组分A和B的总和中的比例为0.5重量%-15重量%,
并且其中填料的比例为2.5重量%-6重量%,基于聚酰胺组分和填料的总质量;
其中至多10mol%的PA均聚物可以由其他酰胺形成单元形成;
其中至多10mol%的二胺残基(DA')可以被仅具有一个氨基末端或仅具有一个羟基末端的聚醚取代。
2.根据权利要求1所述的模塑料,其中基于PA共聚物的总质量,组分B的PA共聚物具有8重量%-30重量%的聚醚含量。
3.根据权利要求1和2中任一项所述的模塑料,其中所述聚醚具有不超过5000g/mol的数均分子量Mn。
4.根据权利要求1至3中任一项所述的模塑料,其中对于酰胺形成单元中的碳原子数,所述聚酰胺组分的PA共聚物的链长和PA均聚物的链长彼此相差平均不超过10%,其中所述差基于所述链长的较高值。
5.根据权利要求1至4中任一项所述的模塑料,其特征在于,所述模塑料的结晶度低于包括等量的相同组分A和用于增加导电性的填料的混合物的结晶度,其中所述模塑料的任何其他成分在种类和量上同样相同。
6.根据权利要求1至5中任一项所述的模塑料,其特征在于,其不含增塑剂。
7.根据权利要求1至6中任一项所述的模塑料用于制备中空型材的用途。
8.单层或多层中空型材,其具有至少一个由根据权利要求1至6中任一项所述的模塑料组成的层。
9.根据权利要求8所述的单层或多层中空型材,其具有至少一个阻隔层。
10.根据权利要求8和9中任一项所述的单层或多层中空型材,其中设置在中空体中的所述阻隔层的内侧上的层不含增塑剂。
11.用于制备根据权利要求1至6中任一项所述的模塑料的方法,其特征在于,通过熔融混合来混合各成分。
12.根据权利要求11所述的方法,其特征在于,成分A和B以及填料同时彼此混合。
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