CN114321520A - 具有聚酰胺外层的多层管的组成和制造方法 - Google Patents
具有聚酰胺外层的多层管的组成和制造方法 Download PDFInfo
- Publication number
- CN114321520A CN114321520A CN202111084741.9A CN202111084741A CN114321520A CN 114321520 A CN114321520 A CN 114321520A CN 202111084741 A CN202111084741 A CN 202111084741A CN 114321520 A CN114321520 A CN 114321520A
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- China
- Prior art keywords
- layer
- polypropylene
- multilayer tube
- tube
- polyamide
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- Pending
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Images
Classifications
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Abstract
本公开提供了一种多层管,其包括聚酰胺外层、聚烯烃中间层和热塑性弹性体内层。聚酰胺外层提供足够的机械强度,聚烯烃中间层保护聚酰胺不与水接触以避免水解降解。热塑性弹性体内层可防止聚烯烃中间层出现应力开裂,并为连接提供出色的密封。
Description
技术领域
本公开涉及一种用于机动车辆中的管。更具体地,本公开涉及一种多层管,其可用于运输流体以在机动车辆中进行温度控制。
背景技术
已经提出将诸如塑料和弹性体的合成材料的单层和多层管用于冷却剂管线。电动和机动车辆的冷却剂管线需求不断增长。电动车辆和具有内燃机的机动车辆的冷却系统类似。两者都通过一系列热交换管循环冷却剂,以将热量从发动机中转移出去。
中温冷却剂系统在约90℃至约120℃的连续温度下运行,峰值温度比连续温度高约5℃至约10℃。重要的是,构成冷却剂管的材料应能在运行温度范围内防止冷却剂扩散和泄漏。管必须在运行温度范围内具有良好的抗蠕变性,并在与其他管连接时表现出良好的环向强度,以避免在应力点发生泄漏。管还必须在运行期间保持其爆破压力强度,同时在更高的压力下运输冷却剂。最后,管应该具有足够的密封性,用于连接到系统的组件或连接到其他管,通常是通过包括倒钩连接在内的装配连接。
寻找具有所有这些特性并且同时经济的材料是一个挑战。多层管可用于提供单个管中的所有基本特性。通常,最成功的多层管是采用由耐外部环境的材料组成的外层共挤出的。最内层选择由一种能够以低成本阻止冷却剂扩散,同时表现出长期适用性的材料组成。
由聚酰胺外层和聚烯烃内层制成的多层冷却剂管已被使用。聚酰胺提供良好的机械和化学性能,包括在相对较高温度下的高爆裂强度。然而,一些聚酰胺在冷却剂/水环境中可能具有相对较弱的抗水解性。聚烯烃内层通过保护聚酰胺外层免受管中输送的水的影响,从而保护其免受水解降解。
聚烯烃内层可能具有降低的抗蠕变应力开裂性。据报道,聚丙烯会形成微裂纹,使冷却液泄漏到聚酰胺外层。然后发生的水解降低了其爆破强度,这可能导致管道故障或连接处泄漏。
一个目的是提供一种低成本的多层管,其将在中等连续温度范围内在机动车辆中特别地输送流体。
发明内容
本公开提供了一种多层管10及其制造方法,所述多层管10包括聚酰胺外层18、聚烯烃中间层16和热塑性弹性体内层14。聚酰胺外层18提供足够的机械强度和环境保护,聚烯烃中间层16保护聚酰胺不与水接触以避免水解降解并防止冷却剂扩散和渗透。热塑性弹性体内层14作为与水性冷却剂环境的极好界面材料并防止聚烯烃中间层16中的应力开裂并为连接提供极好的密封。
附图说明
下面结合附图对本发明的一个或多个示例性实施方案进行描述,其中:
图1是根据本公开的具有三层的管的平面图;
图2是穿过图1的管的截面图。
图3是穿过图2的管的替代实施方案的截面图。
图4是制造本公开的管的方法的示意图。
具体实施方式
本公开是图1和图2所示的多层管10。多层管是中温冷却剂管线应用的理想选择,但也可用于其他应用。管10具有至少一个内层或第一层14、至少一个中间层或第二层16以及至少一个第三层或外层18。管10可具有聚酰胺外层18、聚烯烃中间层16和热塑性弹性体内层14。聚酰胺外层18提供足够的机械强度并且聚烯烃中间层16保护聚酰胺不与水接触以避免水解降解。本公开提出热塑性弹性体内层14以防止聚烯烃中间层16中的蠕变应力裂纹并提供与连接器或其他管的优良密封。
多层管10优选地通过在常规共挤出工艺中同时共挤出热塑性材料来制造。管10可以被共挤出到合适的长度,或者可以以连续的长度共挤出并随后切割以适合给定的应用。本公开的管10可具有至多约50mm的外径和约5mm至约30mm的内径。总壁厚可为0.5至约7mm,合适地约0.9至约4mm,优选1至约3mm。管也可以具有光滑的孔或波纹表面。
管10可用于在电动车辆和内燃机车辆中的发动机的中温冷却剂输送。通常,冷却剂将是基于二醇的水性冷却剂,例如乙二醇。管10通常可能会遇到在约1至4巴最大表压下的约90℃至约120℃的连续温度应用以及约125℃至约135℃的峰值温度。
管10包括内层14。内层14可以主要包括热塑性弹性体材料,该材料因其柔韧性和连接密封性而被选择。如本文所用,术语“主要的”或“占优势的”是指大于50%,适当地大于75%,优选地大于90%。管10的内层14可以容纳摩擦配合连接,例如多倒钩阳连接器。内层必须具有围绕插入管中的多倒钩阳连接器密封地符合的特性,以建立在管10的整个寿命期间持续的流体密封连接。内层可以具有约0.1至约1mm的壁厚,优选约0.1至约0.7mm。
适用于内层14的材料是热塑性弹性体(TPE)。TPE包含热塑性材料的主相和弹性体或橡胶的次相。TPE具有热塑性材料的特性,但硬度更像橡胶。粘附到中间层16的TPE是最合适的。合适的TPE包括热塑性橡胶,其为由苯乙烯-乙烯/丁烯-苯乙烯嵌段共聚物和聚氯乙烯复合物与增塑剂组成的组合物。
优选的TPE主要是热塑性硫化橡胶(TPV)。TPV是一种大部分完全固化的乙烯-丙烯二烯单体(EPDM)颗粒封装在聚丙烯基质中的硫化合金。聚丙烯基质构成主相,乙烯-丙烯二烯单体构成次相。TPV可从各种供应商处商购获得,包括在SANTOPRENE产品线下,一种热塑性橡胶组合物,来自ExxonMobil Chemical,Irving,Texas和SARLINK产品线,一种耐油热塑性组合物,可从Teknor Apex of Pawtucket,Rhode Island商购获得。TPV也可从ElastronGroup获得,其在Kocaeli,Turkey制造。基于ISO 868,优选的TPV应具有约55至约95,优选地约80至约90的肖氏A硬度。不具有EPDM相的热塑性材料,例如聚丙烯将具有更大的肖氏A硬度。如果需要,可以对这些材料进行改性以包括阻燃剂、增塑剂和其他类似添加剂。
在一个实施方案中,中间层16可以主要包括可熔融加工的聚烯烃材料。聚烯烃材料提供足够的防水屏障以保护聚酰胺外层18免于水解。合适的聚烯烃材料是聚丙烯。因此,中间层可主要包含聚丙烯。聚丙烯具有优异的抗渗透性。如果内层14是具有包含聚丙烯的主相的TPE,则聚丙烯是特别合适的,以实现相互粘合特性。聚丙烯材料可包括丙烯均聚物或丙烯共聚物。聚丙烯共聚物包含与至少另一种烯烃单体聚合的丙烯。其他烯烃单体可以是具有不超过四个碳原子的取代或未取代的烯烃、乙烯醇或乙酸乙烯酯,以及它们的混合物。在共聚物中,聚丙烯与聚合物链中的其他烯烃单体共价键合。
聚丙烯均聚物或共聚物可以通过任何已知的方法制造。例如,丙烯聚合物可以在齐格勒-纳塔催化剂体系或茂金属催化剂体系存在下由丙烯单体制备。可以类似地制造嵌段共聚物,不同的是丙烯通常首先在第一反应器阶段中单独聚合或与另一种烯烃单体聚合以形成半结晶基质,然后在第二阶段或后续阶段中在第一反应器中产生的聚合物存在下丙烯的低结晶度或无定形链段和其他烯烃单体共聚。所述其他烯烃单体应具有不超过四个碳原子,优选乙烯。商业聚丙烯无规和嵌段共聚物可从多个聚丙烯生产商处广泛获得,包括各种等级。优选无规聚丙烯共聚物。
丙烯的无规共聚物可包含以无规方式插入的共聚单体,从而破坏主链结晶度,导致共聚物的熔点从均聚丙烯的约165℃降至无规共聚丙烯中的低至约130℃,取决于所用共聚单体的数量和类型。
聚丙烯的共聚物可以在多步方法中共聚以获得嵌段共聚丙烯,其中链段由相对结晶的均聚丙烯或无规共聚丙烯组成和链段由相对无定形或低结晶度的丙烯乙烯共聚物组成。嵌段共聚物的熔点将由共聚物的结晶度更高的链段支配,以给出均聚丙烯嵌段共聚物的约165℃或无规共聚丙烯嵌段共聚物的更低的熔点。
乙烯是聚丙烯共聚物的优选共聚单体,但其他烯烃单体可以是合适的。此外,无规共聚丙烯优于嵌段共聚丙烯。丙烯共聚物中共聚单体,特别是乙烯的质量分数应该在约0.1重量%和约15重量%之间,优选在约0.2重量%和约6重量%之间。
多层管10可具有主要包含聚酰胺的外层18。可以使用的聚酰胺是脂肪族均缩聚物和共缩聚物,例如PA46、PA66、PA68、PA610、PA612、PA410、PA810、PA1010、PA412、PA1012、PA1212、PA6、PA7、PA8、PA9、PA10、PA11和PA12。聚酰胺的名称符合国际标准,其中第一位数字表示起始二胺中的碳原子数,后一位数字表示二羧酸中的碳原子数。如果仅给出一个数字,则表示已使用α,ω-氨基羧酸或由其衍生的内酰胺作为起始材料;否则,可参考H.Domininghaus,DieKunststoffe und ihre Eigenschaften,第272页及随后各页,VDI-Verlag,1976。
脂肪族PA612的使用是特别优选的,因为这种聚酰胺在高使用温度下具有高爆破强度,其次具有令人满意的尺寸稳定性和对来自环境的化学侵蚀的优异耐受性。例如,PA612在干燥条件下可具有620MPa的弯曲模量。如果使用共聚酰胺,它们可以包括例如己二酸、癸二酸、辛二酸、间苯二甲酸、对苯二甲酸、萘-2,6-二羧酸等作为共酸和双(4-氨基环己基)甲烷,三甲基六亚甲基二胺、六亚甲基二胺等作为共二胺。内酰胺如己内酰胺或月桂内酰胺和氨基羧酸如11-氨基十一烷酸同样可以作为共组分并入。
其他合适的聚酰胺是混合的脂族/芳族缩聚物。
聚酰胺组合物可包含这些聚酰胺中的一种或多种作为混合物。此外,可以存在至多50重量%的其他热塑性材料,只要这些不会损害粘合能力。可以存在的其他热塑性材料特别是增加冲击韧性的橡胶,例如乙烯-丙烯或乙烯-丙烯-二烯共聚物、聚烯烃、聚戊烯、聚辛烯、烯基芳族化合物与脂族烯烃或二烯的无规或嵌段共聚物或具有玻璃化转变温度Tg<-10℃的(甲基)丙烯酸酯、丁二烯或丁苯橡胶的核壳橡胶,其中核能够交联并且壳能够由苯乙烯和/或甲基丙烯酸甲酯和/或其他不饱和单体组成。
聚酰胺优选具有过量的氨基端基,这通常是由于在制备中使用二胺作为分子量调节剂而产生的。氨基端基过量也可以通过混合氨基含量低的聚酰胺和氨基含量丰富的聚酰胺来获得。氨基端基与羧基端基的比率则应为至少51:49,优选至少55:45,特别优选至少60:40,尤其是至少70:30。
此外,聚酰胺还可包含相对少量的用于设置特定性能所需的添加剂。实例是颜料或填料如炭黑、二氧化钛、硫化锌、硅酸盐或碳酸盐,加工助剂如蜡、硬脂酸锌或硬脂酸钙,阻燃剂如氢氧化镁、氢氧化铝或三聚氰胺氰尿酸盐,玻璃纤维,抗氧化剂,紫外线稳定剂和赋予产品抗静电性能或导电性的添加剂,例如碳纤维、石墨原纤维、不锈钢纤维或导电炭黑。
在一个具体实施方案中,聚酰胺组合物可包含1至25重量%,特别优选2至20重量%,尤其是3至15重量%的增塑剂。适合作为增塑剂的常规化合物是例如在醇组分中具有2至20个碳原子的对羟基苯甲酸酯或在胺组分中具有2至12个碳原子的芳基磺酸的酰胺,优选苯磺酸的酰胺。可能的增塑剂是例如对羟基苯甲酸乙酯、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。外层18可具有约0.1至约1mm,优选约0.1至约0.8mm的壁厚。
内层14可以在挤出过程中与其他层共挤出,或者其他层可以在随后的过程中围绕内层挤出,例如通过十字头挤出。外层18可以在挤出过程中与其他层共挤出,或者可以在随后的过程中围绕其他层挤出,例如通过十字头挤出。
为了在包含聚烯烃的中间层16和包含聚酰胺的外层18之间获得强粘合,可以使用粘合层。如图3所示,管20可以具有介于中间层16和外层18之间的粘合层22。在一个可能的实施方案中,中间层16的材料是粘合改性的,例如,通过掺入酸酐基团。中间层16的材料也可以作为未改性聚丙烯类型与改性丙烯类型的混合物存在。在第二个可能的实施方案中,中间层16由两个子层组成,其中与聚酰胺层相邻的一个子层是粘合改性的,而另一个子层不必进行粘合改性。除了粘合改性之外,这里可以使用不同的聚丙烯模塑组合物作为层材料。在另一个可能的实施方案中,具有不同组成的粘合层22位于中间层16和外层18之间。在这方面,可以使用例如聚酰胺/聚丙烯共混物,其中聚丙烯组分的至少一部分是粘合改性的。
在中间层16和内层14之间不需要使用粘合层。我们已经发现,TPE的内层14,尤其是TPV,可能不需要粘合层并且可以直接粘合到聚烯烃中间层16,如图2和3所示。主要包含聚丙烯的TPE的内层12特别地粘合到主要包含聚丙烯的中间层。在一个实施方案中,具有主要包含聚丙烯的主相和主要包含EPDM的次相的TPV与主要包含聚丙烯的中间层16很好地结合。
较高共聚单体丙烯-α-烯烃共聚物基粘合剂可以用作粘合层22。用于粘合层22的合适粘合剂可以是聚丙烯基粘合剂。优选的聚丙烯基粘合剂是酸酐改性的聚丙烯树脂。每个粘合层22可具有约0.05至约0.5mm,优选约0.05至约0.2mm的壁厚。
本发明的管10适用于机动车辆并且可以包括外层18,该外层不与外部环境发生反应并且可以承受各种冲击、振动疲劳和温度变化以及暴露于在机动车的正常运行过程中会接触到的各种腐蚀性或降解性化合物。适用于本发明的材料可由任何可熔融加工的可挤出热塑性材料组成,这些材料可抵抗紫外线降解和热的极端变化。选择的材料还可以表现出对环境危害的抵抗力,例如暴露于道路盐、氯化锌和CaCl2,以及在与发动机油和制动液等材料接触时抵抗降解。
现在参照图4,示出了生产本公开的管10的方法的示意图100。该方法包括同时至少挤出包含热塑性弹性体材料的内层14、围绕内层的包含聚烯烃材料的中间层16和围绕中间层的包含聚酰胺材料的外层18的步骤。挤出通过挤出机102进行,以将聚合物材料挤出成合适的管状结构,该结构至少包括内层14、中间层16和外层18。一个或更少的挤出机102、104、106、108和/或110可用于要挤出的每一层。如果需要,也可以在中间层16和外层18和/或内层14之间挤出一层或多层粘合层。应当理解,可以根据需要使用更少或任意数量的挤出机。如果使用多于一个挤出机,则材料然后通过共挤出头112。然后该方法包括通过例如水箱114进行骤冷的步骤。然后共挤出管10通过拉拔器116送出,之后通过切割器122将管切割成所需长度。
多层管10具有汽车冷却剂运输所需的强特性。预计管10在-40℃下能承受1.5J(2ft-lbs)力的冲击,并且表现出比传统聚酰胺管更好的抗冷却剂渗透性。管10能够制成波纹管而不会分层,并且具有足够的抵抗在典型操作期间将遇到的爆裂压力的能力,并且还能够承受在制造和测试期间将遇到的真空压力。该管还具有足够的密封能力和环向强度,使其能够与带倒钩的连接(barbed connection)结合而不会泄漏。
虽然下面结合具体实施例进行描述,但是应当理解,该描述旨在说明而不是限制前述描述和所附权利要求的范围。
无需进一步详述,相信本领域技术人员可以在不脱离本发明的精神和范围的情况下,最大限度地利用本发明并容易地确定本发明的基本特征,利用前述描述,对本发明进行各种改变和修改,使其适应各种用途和条件。因此,前述优选的具体实施例应被解释为仅是说明性的,而不以任何方式限制本公开的其余部分,并且旨在涵盖包括在所附权利要求的范围内的各种修改和等效布置。
在上文中,除非另有说明,否则所有温度均以摄氏度表示,并且所有份数和百分比均以重量计。
Claims (20)
1.一种多层管,包括:
包含热塑性弹性体的内层;
包含聚烯烃的中间层;和
包含聚酰胺的外层。
2.根据权利要求1所述的多层管,其中所述内层包含热塑性硫化橡胶。
3.根据权利要求2所述的多层管,其中所述内层包含聚丙烯主相和弹性体次相。
4.根据权利要求3所述的多层管,其中所述弹性体次相包括乙烯-丙烯二烯单体橡胶。
5.根据权利要求1所述的多层管,其中所述中间层包含聚丙烯。
6.根据权利要求5所述的多层管,其中聚丙烯为均聚物。
7.根据权利要求5所述的多层管,其中聚丙烯为共聚物。
8.根据权利要求7所述的多层管,其中聚丙烯共聚物包括乙烯共聚物。
9.根据权利要求1所述的多层管,还包括位于中间层和外层之间的粘合层。
10.根据权利要求8所述的多层管,其中所述粘合层为聚丙烯基粘合剂。
11.根据权利要求1所述的多层管,其中所述外层为尼龙612、610或12。
12.一种多层管,包括:
包含热塑性弹性体的内层;
包含聚丙烯的中间层;和
包含聚酰胺的外层。
13.根据权利要求11所述的多层管,其中所述内层和所述中间层中的至少一个包含聚丙烯共聚物。
14.根据权利要求12所述的多层管,其中所述内层包含聚丙烯共聚物主相和弹性体次相。
15.根据权利要求14所述的多层管,其中所述弹性体次相包括乙烯-丙烯二烯单体橡胶。
16.根据权利要求12所述的多层管,其中所述中间层包含丙烯共聚物与乙烯共聚物。
17.根据权利要求1所述的多层管,其中所述外层为尼龙612、610或12。
18.一种制造多层管的方法,包括:
挤出包含热塑性弹性体的内层、围绕所述内层的包含聚烯烃的中间层和围绕所述中间层的包含聚酰胺的外层;其中所有层同时挤出。
19.根据权利要求20所述的方法,还包括同时挤出在中间层和外层之间的粘合层。
20.根据权利要求20所述的方法,其中所述内层为热塑性硫化橡胶。
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US17/037,248 US20220097276A1 (en) | 2020-09-29 | 2020-09-29 | Composition of a multi-layer tube with a polyamide outer layer and process for making |
US17/037248 | 2020-09-29 |
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CN114321520A true CN114321520A (zh) | 2022-04-12 |
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DE102004036179A1 (de) * | 2004-07-26 | 2006-03-23 | Degussa Ag | Kühlmittelleitung |
FR2876765B1 (fr) * | 2004-10-19 | 2007-01-19 | Nobel Plastiques Soc Par Actio | Tube multicouche tpe/pp/renfort |
WO2007032033A1 (en) * | 2005-09-16 | 2007-03-22 | Dayco Fluid Technologies S.P.A. | Multi-layer piping for conveying and heating a fluid |
DE102006011493A1 (de) * | 2006-03-14 | 2007-09-20 | Degussa Gmbh | Druckluftbremsleitung |
DE102018213140A1 (de) * | 2018-08-06 | 2020-02-06 | Aft Automotive Gmbh | Mehrschichtverbund sowie Fluidleitung |
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