CN103153604B - 结构复合层压板 - Google Patents
结构复合层压板 Download PDFInfo
- Publication number
- CN103153604B CN103153604B CN201180022580.9A CN201180022580A CN103153604B CN 103153604 B CN103153604 B CN 103153604B CN 201180022580 A CN201180022580 A CN 201180022580A CN 103153604 B CN103153604 B CN 103153604B
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- Prior art keywords
- coat
- structural foam
- composite laminate
- foam
- dyne
- Prior art date
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- Y10T428/249953—Composite having voids in a component [e.g., porous, cellular, etc.]
- Y10T428/249987—With nonvoid component of specified composition
- Y10T428/249991—Synthetic resin or natural rubbers
Abstract
本发明涉及密封、隔阻和结构加固的层压板结构。更具体地,本发明涉及包括结构泡沫和载体材料的层压板结构。
Description
优先权声明
本申请要求美国临时申请第61/310,580号(2010年3月4日提交)的提交日的权利,所述申请全部内容在此以引用的方式纳入本说明书。
技术领域
本发明总体涉及密封、隔阻和结构加固的层压板结构。更具体地,本发明涉及包括结构泡沫和载体材料的层压板结构。
背景技术
车辆舱室的结构加固通常通过将聚合物载体塑模成反映需要加固的舱室轮廓的具体形状,并将可膨胀泡沫材料置于载体的特定表面上而实现。因此,各载体必须定制成特定形状,这需要形成和使用多个模具,还需要既耗时又昂贵的注模过程。许多载体需要过度塑模或多次注模以形成正确的形状和加固目的所需的足够密度。在尝试降低生产载体有关的成本和工作量的过程中,已尝试提供不包括载体的可膨胀泡沫材料作为结构泡沫。优点在于结构泡沫的大小和形状可以快速改变并定制成任何需要的形状。遗憾的是,在没有载体的情况下,仅包括结构泡沫的加固元件的强度降低。此外,没有载体则难以控制结构泡沫的膨胀。因此希望提供一种加固结构,其具有单独的结构泡沫的定制优点,但仍能提供舱室加固所必需的强度。还希望载体使所得结构仅增加最少的重量和成本,但仍能提供与单独的结构泡沫或载体可实现的相比改进的强度和加固能力。
发明内容
本发明通过提供一种复合层压板结构而满足上述部分或全部需求,所述复合层压板结构具有加固层和结构泡沫,以使加固层和结构泡沫之间形成的结合提供超过单独的结构泡沫或加固层的强度。本发明涉及一种形成为结构提供密封、隔阻或加固的复合层压板的方法,所述方法通过提供加固层以及将环氧基可膨胀结构泡沫置于其上而进行。加固层可具有至少为约35达因/cm的表面张力。结构泡沫和加固层的表面张力在彼此的约15达因/cm以内。加固层和结构泡沫的表面张力为负荷从结构泡沫转移至加固层提供足够的润湿,以便增加复合层压板的拉伸强度并增加复合层压板的搭接剪切强度。
本发明还涉及一种为结构提供密封、隔阻或加固的复合层压板,其包括加固层和环氧基可膨胀结构泡沫。加固层可具有至少为约35达因/cm的表面张力。将环氧基可膨胀结构泡沫材料置于加固层上以形成复合层压板。结构泡沫和加固层的表面张力在彼此的约15达因/cm以内以便改善结构泡沫和加固层之间的粘合性。
本发明还涉及一种形成复合层压板的方法,所述方法通过提供聚合加固层以及通过共挤压过程将环氧基可膨胀结构泡沫材料置于加固层上从而形成复合层压板而实现。随后将复合层压板暴露于高于150℃的温度。加固层具有至少为约35达因/cm的表面张力且可包括至少一个可自由反应的化学官能团,如羧酸或伯或仲胺。结构泡沫可包括环氧树脂、包含约1∶3至3∶1份环氧(epoxy)与弹性体的环氧/弹性体加合物、以及芯/壳聚合物抗冲改性剂。在暴露于高于150℃的温度时,环氧树脂可与加固物(例如与加固层的羧酸或胺)形成共价键。共价键允许负荷从结构泡沫转移至加固层以便增加复合层压板的拉伸强度。
复合层压板与用于密封、隔阻和加固舱室的现有结构和材料相比包括改善的物理性能。这些改善的物理性能可包括但不限于,与使用单独的结构泡沫相比,提高的垂直上升量(verticalrise)、改善的搭接剪切强度、增加的拉伸和弯曲性能以及提高的T-剥离强度。本发明的结构还可具有改善的储存和运输稳定性以及改善的储藏寿命。本文公开的结构还可定制结构的大小、形状以及泡沫膨胀方向,因为载体容易控制。此外,载体的存在使得与使用单独的结构泡沫相比可改善对结构泡沫膨胀的控制。
附图说明
图1是本文教导的说明性层压板结构的截面图。
图2示出结构泡沫A、B、C和D的垂直上升量的图示,以具有或不具有加固层表示。
图3示出结构泡沫A、B、C和D的搭接剪切强度的图示,以具有或不具有加固层表示。
图4示出结构泡沫A、B、C和D的弯曲强度的图示,以具有或不具有加固层表示。
图5示出结构泡沫A、B、C和D的弯曲模量的图示,以具有或不具有加固层表示。
图6示出结构泡沫A的弯曲测试负荷位移曲线的图示,以具有或不具有加固层表示。
图7示出结构泡沫B的弯曲测试负荷位移曲线的图示,以具有或不具有加固层表示。
图8示出结构泡沫C的弯曲测试负荷位移曲线的图示,以具有或不具有加固层表示。
图9示出结构泡沫D的弯曲测试负荷位移曲线的图示,以具有或不具有加固层表示。
具体实施方式
概言之,本文的教导提供一种层压板结构,其包括至少加固层和位于其上的结构泡沫材料。例如,图1示出具有加固层10和位于加固层两个表面上的结构泡沫层12。加固层为结构泡沫材料提供支撑机制,借此在加固层与结构泡沫之间形成结合,以便发生从结构泡沫至加固层的负荷转移。加固层和结构泡沫两者的表面张力可以相似(例如匹配)以便强化加固层与结构泡沫之间的结合。加固层和结构泡沫之间强化的结合使得层压板具有一种或多种以下特征:改善的剥离强度、改善的拉伸性能、改善的搭接剪切性能、改善的压缩性能、改善的垂直上升量、以及改善的弯曲性能。
加固层和结构泡沫之间的结合可由多种方法形成。例如,加固层的表面张力和结构泡沫的表面张力可以相匹配以便提高加固层和结构泡沫之间的结合。随着润湿容易性的增加,观察到改善的结合。本发明显示出的优越的机械和结构性能要求结构泡沫对加固层的粘合性增加,以便置于所得复合层压板上的负荷可由粘合剂转移至加固层,从而支撑部分或基本全部的负荷。因此,确保改善的粘合性所依赖的一个技术是通过匹配粘合剂和加固层的表面张力以便改善润湿。
为了实现结构泡沫和加固层之间提高的结合强度,加固层和结构泡沫两者的表面张力可为至少约35达因/cm。加固层和结构泡沫二者的表面张力可以小于约80达因/cm。如果加固层的表面张力下降至低于35达因/cm,则可以处理加固层以提高其表面张力。即使当加固层的表面张力等于或大于35达因/cm时,仍然可以处理加固层从而改变其表面张力以与结构泡沫的表面张力匹配。本文记载了处理加固层从而改变其表面张力的方法。例如,结构泡沫可包括提供约47达因/cm的表面张力的环氧树脂。因此,为了改善与结构泡沫的结合强度,加固层的表面张力为至少约38达因/cm,但优选至少约42达因/cm,或更大。
结构泡沫优选包括环氧树脂。本文使用的环氧树脂意指任何含有至少一个环氧官能团的常规二聚、低聚或聚合环氧材料。环氧树脂可以是双酚A环氧树脂。环氧树脂可构成约2重量%至约80重量%的结构泡沫。环氧树脂可构成约10重量%至约30重量%的结构泡沫。环氧树脂可构成至少约10重量%的结构泡沫。环氧树脂可构成少于约30重量%的结构泡沫。环氧树脂可以是液体或固体环氧树脂或可以是液体和固体环氧树脂的结合物。
结构泡沫还可包括环氧/弹性体加合物。更具体地,加合物基本完全(即,至少70%、80%、90%或更多)由一种或多种在23℃温度下为固体的加合物组成。加合物可构成约5重量%至约80重量%的结构泡沫。加合物可构成至少约5重量%的结构泡沫。加合物可构成至少约10重量%的结构泡沫。加合物可构成少于约70重量%的结构泡沫。加合物可构成少于约30重量%的结构泡沫。加合物本身通常包括约1∶5至5∶1份的环氧与弹性体,更优选约1∶3至3∶1份的环氧与弹性体。示例性弹性体包括,但不限于,天然橡胶、苯乙烯-丁二烯橡胶、聚异戊二烯、聚异丁烯、聚丁二烯、异戊二烯-丁二烯共聚物、氯丁橡胶、丁腈橡胶(例如,丁腈,如羧基封端丁腈(CTBN))、丁基橡胶、聚硫弹性体、丙烯酸系弹性体、丙烯腈弹性体、硅橡胶、聚硅氧烷、聚酯橡胶、二异腈酸酯连接的缩合弹性体、EPDM(乙烯-丙烯二烯橡胶)、氯磺化聚乙烯、氟化烃等。适用于本发明的其他或替代环氧/弹性体或其他加合物的实例公开于美国专利公布文本2004/0204551,其在此就各方面以引用的方式纳入。作为具体实例,结构泡沫可包括约5重量%至约20重量%的CTBN/环氧加合物。
结构泡沫也可包括抗冲改性剂。抗冲改性剂可构成至少约4重量%的结构泡沫。抗冲改性剂可构成至少约10重量%的结构泡沫。抗冲改性剂可构成至少约17重量%的结构泡沫。抗冲改性剂可构成少于约40重量%的结构泡沫。抗冲改性剂可构成约2重量%至约60重量%的结构泡沫。
抗冲改性剂可包括至少一种芯/壳聚合物。如本文使用的,术语芯/壳聚合物描述一种这样的抗冲改性剂,其中其实质部分(例如,大于30重量%、50重量%、70重量%或更多)包括基本完全被第二聚合材料(即,第二或壳材料)包胶的第一聚合材料(即,第一或芯材料)。如本文使用的,第一和第二聚合材料可包括一种、两种、三种或更多种聚合物,它们在一起结合和/或反应(例如,顺序聚合),或者可以是单独或相同芯/壳体系的一部分。芯/壳抗冲改性剂的第一聚合材料、第二聚合材料或两者包括一种或多种热塑性塑料或基本完全(例如,至少70重量%、80重量%、90重量%或更多)由其组成。示例性热塑性塑料包括,但不限于,苯乙烯类(styrenics)、丙烯腈类、丙烯酸酯类、乙酸酯类、聚酰胺类、聚乙烯类等。可能有利的是第一或芯聚合材料的玻璃化转变温度低于23℃,第二种或壳聚合材料的玻璃化转变温度高于23℃,但不是必需的。
有用的芯-壳接枝共聚物的实例是这样的物质:其中含有化合物如苯乙烯、丙烯腈或甲基丙烯酸甲酯的硬质段(hard)接枝于由含有化合物如丁二烯或丙烯酸丁酯的软质段(soft)或弹性体制成的芯上。美国专利3,985,703——其在此以引用的方式纳入——记载了有用的芯-壳聚合物,其芯由丙烯酸丁酯制成,但可基于乙基异丁基、2-乙基己基或其他烷基丙烯酸酯或其混合物。芯聚合物也可包括其他含有化合物如苯乙烯、乙酸乙烯酯、甲基丙烯酸甲酯、丁二烯、异戊二烯等的可共聚物。壳部分可由甲基丙烯酸甲酯和任选地其他烷基的甲基丙烯酸酯(如乙基、丁基、或其混合的甲基丙烯酸酯)聚合。芯-壳接枝共聚物的实例包括,但不限于,“MBS”(甲基丙烯酸酯-丁二烯-苯乙烯)聚合物,其通过在聚丁二烯或聚丁二烯共聚物橡胶存在下聚合甲基丙烯酸甲酯而制备。MBS接枝共聚物树脂通常具有苯乙烯丁二烯橡胶芯以及丙烯酸系聚合物或共聚物的壳。其他有用的芯-壳接枝共聚物树脂的实例包括,ABS(丙烯腈-丁二烯-苯乙烯)、MABS(甲基丙烯酸酯-丙烯腈-丁二烯-苯乙烯)、ASA(丙烯酸酯-苯乙烯-丙烯腈)、所有丙烯酸类树脂、SAEPDM(苯乙烯-丙烯腈接枝于乙烯-丙烯二烯单体的弹性体骨架上)、MAS(甲基丙烯酸-丙烯酸橡胶苯乙烯)等,及其混合物。
结构泡沫还可包括一种或多种其他聚合物和/或共聚物材料,如热塑性树塑料、弹性体、塑性体、其结合物等。可适当引入结构泡沫的聚合物包括卤化聚合物、聚碳酸酯、聚酮、聚氨酯、聚酯、硅烷、砜、烯丙基类、烯烃、苯乙烯类、丙烯酸酯、甲基丙烯酸酯、环氧树脂、聚硅氧烷、酚醛塑料、橡胶、聚苯醚、邻苯二甲酸酯、乙酸酯(例如,EVA)、丙烯酸酯、甲基丙烯酸酯(例如,乙烯甲基丙烯酸酯聚合物),或其混合物。其他可能的聚合材料可以是或可包括,但不限于,聚烯烃(例如,聚乙烯、聚丙烯)、聚苯乙烯、聚丙烯酸酯、聚(环氧乙烷)、聚(吖丙啶)、聚酯、聚氨酯、聚硅氧烷、聚醚、聚膦嗪、聚酰胺、聚酰亚胺、聚异丁烯、聚丙烯腈、聚(氯乙烯)、聚(甲基丙烯酸甲酯)、聚(乙酸乙烯酯)、聚(偏二氯乙烯)、聚四氟乙烯、聚异戊二烯、聚丙烯酰胺、聚丙烯酸、聚甲基丙烯酸酯。
作为具体实例,结构泡沫可包括至少约2%但少于约15%的热塑性聚醚。结构泡沫可包括至少约10重量%的聚氯乙烯。结构泡沫可包括少于约30重量%的聚氯乙烯。结构泡沫可包括至少约0.1重量%且少于约5重量%的聚环氧乙烷。结构泡沫可包括至少约1重量%的乙烯共聚物(其可以是EVA或EMA共聚物)。结构泡沫可包括至少约15重量%的乙烯共聚物。结构泡沫可包括少于约40重量%的乙烯共聚物。结构泡沫可包括至少约5重量%的丙烯腈。结构泡沫可包括至少约20重量%的丙烯腈。结构泡沫可包括少于约50重量%的丙烯腈。
结构泡沫也可包括多种发泡剂、固化剂和填料。合适的发泡剂的实例包括偶氮二碳酰胺、二亚硝基五亚甲基四胺、4,4i-氧-双-(苯磺酰肼)、三肼基三嗪和N,Ni-二甲基-N,Ni-二亚硝基对苯二甲酰胺。还可在可活化材料中加入发泡剂的促进剂。可以使用多种促进剂以提高发泡剂形成惰性气体的速率。一种优选的发泡剂促进剂是金属盐,或氧化物,例如金属氧化物,如氧化锌。其他优选的促进剂包括改性和未改性的噻唑类或咪唑类。
合适的固化剂的实例包括选自以下的材料:脂族或芳族胺或其各自的加合物、酰胺基胺、聚酰胺、脂环族胺、酸酐、聚羧酸聚酯、异氰酸酯、酚基树脂(例如,苯酚或甲酚酚醛清漆树脂、共聚物如酚萜、聚乙烯苯酚或双酚A甲醛共聚物的那些、双羟苯基烷烃等)、或其混合物。特别优选的固化剂包括改性和未改性的聚胺或聚酰胺,如三亚乙基四胺、二亚乙基三胺、四亚乙基五胺、氰基胍、二氰胺等。也可以提供固化剂的促进剂(例如,改性或未改性的脲,如亚甲基二苯基二脲、咪唑或其结合物)用于制备结构泡沫。
合适填料的实例包括二氧化硅、硅藻土、玻璃、粘土(例如,包括纳米粘土)、滑石、颜料、着色剂、玻璃珠或泡状物、玻璃、碳或陶瓷纤维、尼龙或聚酰胺纤维(例如Kevlar)、抗氧化剂等。这类填料(特别是粘土)可帮助可活化材料在材料流动过程中自流平。可用作填料的粘土可包括选自高岭土、伊利石、绿泥石、蒙脱石或海泡石的粘土,其可焙烧。合适填料的实例包括,但不限于,滑石、蛭石、叶蜡石、锌蒙脱石、滑石粉、囊脱石、蒙脱石或其混合物。粘土也可包括少量其他成分,如碳酸盐、长石、云母和石英。填料也可包括氯化铵,如二甲基氯化铵和二甲基苄基氯化铵。也可使用二氧化钛。一种或多种矿物或石类填料如碳酸钙、碳酸钠等可用作填料。在另一优选实施方案中,硅酸盐矿物如云母可用作填料。优选地,填料包括通常与可活化材料中存在的其他组分不反应的材料。虽然填料可通常存在于可活化材料中而以相对低的重量占据空间,但预期填料也可赋予可活化材料以例如强度和抗冲击性等性能。
可作为结构泡沫而包括的材料的实例包括公开于美国专利7,892,396和7,125,461,以及美国专利申请2004/0204551、2007/0090560、2007/0101679、2008/0060742和2009/0269547的那些,这些文件在此就各个方面以引用的方式纳入本说明书。
加固层包括任何具有结合至结构泡沫所必须的能力的基本为固体的材料。如前文所述,加固层的表面张力优选等于或大于35达因/cm,并且还与结构泡沫的表面张力匹配(例如,相似)。表面张力低于该阈值(或明显高于结构泡沫)的材料也可用作加固层,但必须首先处理以改变材料的表面张力。
可以使用聚合材料作为加固层。某些聚合材料具有与结构泡沫通常使用的环氧基材料的表面张力对应的表面张力值。可用作加固层的聚合材料(不含改变表面张力的处理步骤)的实例可包括,但不限于,缩醛(约47达因/cm)、丙烯酸类树脂(约41达因/cm)、聚酰胺(约41达因/cm)、聚碳酸酯(约46达因/cm)、热塑性或固化的热固性环氧树脂(约46达因/cm)、聚对苯二甲酸乙二酯(约43达因/cm)、聚酰亚胺(约40达因/cm)、聚砜(约41达因/cm)、聚氯乙烯(约39达因/cm)和酚醛塑料(约52达因/cm)。聚酰胺和聚对苯二甲酸乙二酯(PET膜)是用于加固层的两种优选材料。
加固层可包括金属材料,如铝、钢、镁、锡、铁、镍、铜、钛等。加固层可以是不同金属材料的结合物。
临界表面张力低于38达因/cm的那些材料,如果可进行改性以满足表面张力需求,仍可用作本发明的加固层。三种改变基底表面张力的常规方法是:(1)涂布液体底漆(包括使用强酸和/或碱);(2)电晕放电;和(3)用石油基气体和空气混合物燃烧。这些方法通常通过氧化基底表面而成功,从而提高其表面张力。
另一种确保结构泡沫和加固层之间提高的粘合性的机制是共价键合。共价键合通过加固层和结构泡沫之间的化学反应发生。为了形成共价键,复合层压板可能需要暴露于高温(例如,超过150℃的温度)。因此,在制造复合层压板过程中(例如,共挤压过程中),温度通常不升高至形成共价键所需的水平。然而,共价键可以在车辆暴露于这种高温下的车辆油漆烘烤周期中形成。
除了合适的暴露时间和温度,生成共价键的化学反应要求结构泡沫和加固层之间具有适当的化学匹配。结构泡沫本身是多组分化合物,其活性成分包括多种分子量的环氧树脂。环氧树脂可基于双酚A的二缩水甘油醚(DGBA),其一般化学结构可表示为:
环氧树脂的官能组分是环氧化物基团(例如,环氧乙烷环),其位于环氧树脂分子的末端。存在于结构泡沫粘合剂中的环氧树脂具有的环氧重量当量在170至6000g/当量范围内,但更可能在170至2000g/当量范围内,最理想在180至1000g/当量范围内。因此,为了在结构泡沫和加固层之间成键,加固层必须含有将与环氧树脂反应的化学官能团。将与环氧树脂反应的化学官能团的实例包括羟基、羧酸、胺、异腈酸酯和酸酐基团。许多热塑性塑料含有一个或多个这些基团,尤其是当它们是通过缩聚而构建时。缩合热塑性塑料的实例有聚酰胺、聚酯、聚碳酸酯和聚氨酯。
加固层可包括这样的热塑性膜,其含有可在复合层压板的最后烘烤周期之后生成共价化学键的化学官能团。市售的膜通常由缩聚物(如聚酯(例如Mylar)、聚酰胺(尼龙)和聚碳酸酯)制得。
如果使用聚酯膜作为加固层,可以形成聚酯/环氧键。当复合层压板的加固层是聚酯,如聚对苯二甲酸乙二酯时,形成共价键所需的化学反应可在暴露于高温时发生。通常,聚酯树脂为链端由羧酸和醇化学官能二者所封端的高分子量缩聚物。
例如,通常转化为膜的聚酯是聚对苯二甲酸乙二酯(PET)和聚对苯二甲酸丁二酯(PBT)。在这两种情况下,聚合物均由醇和羧酸二者封端。环氧化物基团与聚酯(如聚对苯二甲酸乙二酯(下文示为“PET”))末端上的羧酸的反应如下进行:
环氧化物基团与聚酯(如聚对苯二甲酸乙二酯(下文示为“PET”))末端上的醇的反应如下进行:
与上文示出的环氧化物/聚酯反应相似,复合层压板的加固层可为聚酰胺(PA)(例如,尼龙(聚酰胺-6(PA-6))并因而可引起环氧化合物/聚酰胺反应。通常,聚酰胺为链由羧酸和伯胺化学官能二者所封端的高分子量缩聚物。这些聚合物通常由伯胺和羧酸二者封端。环氧化物基团与聚酰胺(如PA-6)末端上的羧酸的反应以上文关于聚酯所示相同的方式进行。环氧化物基团与聚酰胺(下文示为“PA”)的伯胺的反应如下进行:
在上文所示的环氧/聚酯和环氧/聚酰胺这两种反应中,结构泡沫的环氧部分与加固层的羧酸、醇或胺之间形成共价键。所得复合层压板表现出改善的物理特性,这在本文中确认是基于加固层与结构泡沫之间的结合强度。加固层与结构泡沫之间增大的结合强度使复合层压板的许多物理性能改善。描述这些改进的数据在下文示出。使用结构泡沫的多个实例得到数据,这些结构泡沫确认具有表1示出的组成:
重量% | ||||
成分 | A | B | C | D |
环氧/弹性体加合物 | 15.70 | 15.58 | 15.58 | 14.71 |
环氧化的乙烯共聚物 | 1.95 | 1.93 | 1.93 | 1.74 |
甲基丙烯酸乙二酯 | 1.95 | 1.93 | 1.93 | 8.03 |
填料 | 43.1 | 46.56 | 43.09 | 50.93 |
环氧树脂(固-液混合物) | 17.05 | 14.21 | 16.71 | 9.00 |
多功能苯酚醛清漆环氧树脂 | 2.93 | 2.94 | 2.94 | 3.59 |
固化剂和/或促进剂 | 2.20 | 2.06 | 2.27 | 3.23 |
抗冲改性剂 | 14.1 | 13.98 | 13.98 | 7.36 |
发泡剂 | 0.88 | 0.65 | 1.53 | 1.21 |
颜料 | 0.15 | 0.15 | 0.025 | 0.2 |
加固层和结构泡沫之间增大的结合产生改善的特性,包括结构泡沫膨胀过程中的垂直上升量增加。垂直上升量定义为与结构泡沫膨胀前的厚度相比结构泡沫膨胀时的厚度。加固层起限制结构泡沫横向膨胀的作用,从而使膨胀方向和增加的垂直上升量更可控。垂直上升量的增加与可控的膨胀配合可使结构泡沫与舱室壁更精确地接触并可增加结构泡沫膨胀时的密度,从而改善复合层压板的加固能力。图2包括结构泡沫A、B、C和D的垂直上升量的图示,同时以具有和不具有加固层示出。
将不具有加固层的结构泡沫与包括加固层的结构泡沫相比,加固层和结构泡沫之间改善的结合还使搭接剪切强度改善。增加的搭接剪切强度可提高复合层压板的整体强度,从而改善加固能力。结构泡沫的搭接剪切强度通常直接与体积膨胀有关,较小的泡沫密度(较高的膨胀)会产生较小的搭接剪切强度,并且与结合线(bond-line)有关,较小的结合线产生较高的搭接剪切强度。结合线可定义为粘合剂粘合在一起的两个表面之间的结合间隙或距离。由本发明得到的搭接剪切强度相对于不具有加固层的结构泡沫的改善可归因于泡沫密度的增加,但更明显地来自于加固层有效地将结合线减半。图3包括结构泡沫A、B、C和D的搭接剪切应力图示,以具有和不具有加固层示出。下表2包括垂直上升量和搭接剪切应力的数值结果。
表2
将不具有加固层的结构泡沫与包括加固层的结构泡沫相比,加固层和结构泡沫之间改善的结合还使弯曲强度和弯曲模量改善。弯曲强度和模量根据ASTD790使用3点弯曲测试模型测定。图4和5分别包结构泡沫A、B、C和D的弯曲强度和弯曲模量的图示,以具有和不具有加固层示出。
加固层和结构泡沫之间改善的结合还使能量吸收改善。图6-9包括结构泡沫A(图6)、B(图7)、C(图8)和D(图9)的弯曲测试负荷位移曲线的图示,以具有和不具有加固层示出。
在以下实施例I、II和III中,通过将0.18mm厚的聚对苯二甲酸乙二酯膜置于两片环氧基可膨胀结构泡沫之间来制备复合层压板。这种环氧基可膨胀结构泡沫的一个实例公开于美国专利7,892,396。所得夹层结构于180°F下在热压机中压缩2至3分钟,以使膜形成复合层压板的中间层且整个结构的最终厚度为约3mm。
实施例I
表3提供了纯(neat)状态(例如无加固层)下的和使用聚酯对苯二甲酸酯膜的复合层压板形式的两种环氧基可膨胀结构泡沫性能的比较。所有列出的性能均针对活化后状态下的材料。
表3显示本发明的复合层压板的相对垂直上升量高于纯材料。加固层抑制了活化材料的横向(水平或面内)移动,使得膨胀指向垂直于加固层的平面或轴的方向。
使用3mm结合线和EG-60金属基底,根据ASTMD1002测定搭接剪切强度。表3示出复合结构具有比纯的环氧树脂粘合剂更大的搭接剪切强度。加固层有效减小了表观结合线,产生了更大的搭接剪切强度。
弯曲测试根据ASTMD790使用3点弯曲测试模型完成。使用夹层结构来构建试验样品。顶部和底部基底是0.030″厚的尺寸为1″×6″的EG60钢。结构泡沫填充在中间,得到总厚度(泡沫和钢)为6mm。表3示出复合层压板样品具有比纯的环氧树脂粘合剂更大的弯曲强度和模量。
拉伸测试根据ASTMD638,使用10mm宽、3mm厚的JISK6301-1-MET狗骨结构进行,并以5mm/min的速度测定。在间隔3mm的两个脱模表面之间膨胀泡沫然后在样品仍温热时冲切拉伸棒,由此构建试验样品。含有PET膜的样品使膜沿样品平面取向,以便在张力下膜与样品的其余部分一同被拉伸。表3示出复合层压板样品具有比纯的环氧树脂粘合剂更大的拉伸强度和模量。
表3
实施例II
在本实施例中,复合结构层压板通过将0.18mm厚的聚对苯二甲酸乙二酯膜压制在环氧基可膨胀结构泡沫的片之间而制备。该环氧基可膨胀结构泡沫的一个实例与美国专利No.7,892,396公开的可活化材料相似,不同在于不存在芯/壳聚合物抗冲改性剂。夹层结构于180°F下在热压机中压缩2至3分钟,以使膜基本位于结构的中间且整个结构的最终厚度为约3mm。
表4提供纯状态(不具有加固层)下的和使用聚酯对苯二甲酸酯膜的复合层压板形式的环氧基可膨胀结构泡沫性能的比较。所有列出的性能均针对活化后状态下的材料。
表4
试验细节与实施例I中给出的相同。表4显示复合层压板的所有性能相对于纯的环氧树脂粘合剂都有所改善。
实施例III
根据本发明形成的结构泡沫材料还表现出有利的后活化压缩性能。特别地,使本发明的结构泡沫材料发泡形成样品,然后根据基于ASTMC39的方法测试。虽然本文描述了所述方法,但应理解任何未指明的参数均根据ASTMC39。
形成了三种不同的样品类型。第一种样品通过在气缸(cylinder)或气缸杯(cylindercups)中使纯的(未加固的)环氧基泡沫材料发泡、然后移除从气缸或气缸杯膨胀出的过量泡沫(例如,通过切除从气缸或气缸杯膨胀出的泡沫)而形成。第二种样品通过从平的复合层压板样品上切下圆片并将其堆叠在气缸或气缸杯中以使PET加固层的平面垂直于气缸的轴而构建。然后通过使层状复合层压板在气缸或气缸杯中发泡,而后移除从气缸或气缸杯膨胀出的过量泡沫(例如,通过切除从气缸或缸杯膨胀出的泡沫)来完成该样品。第三种样品通过卷取平的复合层压板样品并使其滑入气缸或气缸杯以使PET加固层的平面平行于气缸的轴而构成。然后通过使层状复合层压板在气缸或气缸杯中发泡,而后移除从气缸或气缸杯膨胀出的过量泡沫(例如,通过切除从气缸或缸杯膨胀出的泡沫)来完成该样品。
测试样品通常发泡至小于1000%、更通常地小于750%、且甚至更通常地小于500%的体积,相对于发泡前的结构泡沫材料的原体积计。这样做可形成高为60mm且直径为30mm的圆柱形样品。随后根据ASTMC39测试圆柱形样品。
表5提供了纯状态下的环氧基可膨胀结构泡沫以及其中PET膜位于垂直于气缸轴和平行于气缸轴的堆叠层中的复合结构层压板的气缸压缩性能的比较。所有列出的性能均针对活化后状态下的材料。
表5
表5显示膜的取向对样品的压缩性能有很大影响,在每种情况下,复合层压板样品的压缩大于纯样品。
可考虑的是,本发明的可活化复合层压板可用作结构粘合材料。在这种实施方案中,复合材料通常被活化和固化(例如,在通常用于电泳或汽车喷漆操作的温度下)以使其粘合至第一元件和第二元件。与第一元件和第二元件的附着面的接触可以在材料的活化和固化之前或过程中发生。结构粘合剂应用的实例公开于美国专利6,887,914和6,846,559,以及美国专利公布文本2004/0204551,所有所述文件在此就各方面以引用的方式纳入本说明书。
在使用复合层压板的过程中,可将一种或多种紧固件或粘合剂附着至复合层压板,以便附着至舱室壁或舱室内的其他位置。紧固件可以是机械紧固件且可包括但不限于,图钉、树形紧固件(treefastener)、铰链、螺钉、机械联锁、一体锁、阳部件(malefeature)、阴部件(femalefeature)、或其任意结合。复合层压板可在复合层压板的每个相对端包括一个图钉。
除了本文公开的复合层压板结构的改善的物理特性之外,与复合层压板相关的制造容易性使其可容易地定制成给定舱室所需的任何形状和大小。复合层压板可共挤压然后容易地改性(例如,冲切、切片)。它们可在配送给客户前或在舱室内组装复合层压板期间现场进行改性。
本文描述的任何数值包括从下限值到上限值之间以一个单位为增量的所有数值,只要任意下限值和任意上限值之间相差至少两个单位。例如,如果述及组分含量或过程变量(如温度、压力、时间等)的值为例如1至90、优选20至80、更优选30至70,则意欲表明数值如15至85、22至68、43至51、30至32等也明确在本说明书中列举出来。对于小于1的数值,一个单位可适当地认为是0.0001、0.001、0.01或0.1。这些仅是具体意欲指出的那些的实例,所列举的最小值和最大值之间数值的所有可能的结合均以相似方式认为在本申请中明确述及。如可知晓的,本文中以“重量份”表示的含量的教导也考虑用于以重量百分比方式表达的相同的范围。例如,在本发明具体实施方式中对范围的表达就“x重量份的所得聚合掺混物组合物”而言也考虑用于教导“x重量%的所得聚合掺混物组合物”的相同所述量的范围。
除非另外指出,所有范围包括两个端点和端点之间的所有数值。与范围相关的“约”或“近似”的使用适用于范围的两个端点。因此,“约20至30”意指涵盖“约20至约30”,包括至少所给的端点在内。
所有文件和参考文献的公开内容(包括专利申请和公布文本)均就各个方面以引用的方式纳入本说明书。描述结合的术语“基本由……组成”应包括指定的元素、成分、组分或步骤,以及不实质上影响结合的基本和新的特征的其他元素、成分、组分或步骤。本文中用于描述元素、成分、组分或步骤的结合的术语“包含”或“包括”的使用也考虑用于基本由元素、成分、组分或步骤组成的实施方案。在本文中使用术语“可”,意指任何描述的“可”包括的属性是任选的。
多个元素、成分、组分或步骤可由单一整合的元素、成分、组分或步骤提供。或者,单一整合的元素、成分、组分或步骤可划分为分开的多个元素、成分、组分或步骤。用于描述元素、成分、组分或步骤的“一个”的公开内容并不意欲排除其他元素、成分、组分或步骤。在本文中所有涉及属于某族的元素或金属指的是CRCPress,Inc.,1989出版并取得版权的元素周期表。任何涉及的族应指该元素周期表中使用lUPAC系统为各族编号所反映的族。
应理解,可以使用本文所述量的浓缩物或稀释物。通常,成分的相对比例仍保持相同。因此,例如,如果教导要求30重量份的组分A和10重量份的组分B,则本领域技术人员应认识到,这种教导也构成以3∶1的相对比例使用组分A和组分B的教导。实施例中浓缩物的教导可在所述数值的约25%(或更高)范围内变化且可预期相似的结果。此外,实施例的这类组成可成功用于本发明方法中。
应理解,以上仅为举例说明。如果需要,其他成分可用于本文公开的任何组合物以实现所需的所得特性。可以使用的其他成分的实例包括抗生素、麻醉剂、抗组织胺药、防腐剂、表面活性剂、抗氧化剂、非结合胆汁酸、防霉剂、核酸、pH调节剂、渗透压调节剂或其任意结合物。
应理解,以上描述旨在说明而非限制。除了实施例之外,多种实施方案以及多种应用在本领域技术人员阅读完上述描述后是显然的。因此本发明的范围不应参照上述记载确定,而是应参照所附权利要求以及这类权利要求所称物质的等同物的完整范围确定。所有文件和参考文献的公开内容(包括专利申请和公布文本)均就各个方面以引用的方式纳入本说明书。本文公开的主题的任何方面在以下权利要求中的省略不是对主题的放弃,也不应被看作是发明人不认为这种主题是公开的本发明主题的一部分。
Claims (22)
1.一种形成为结构提供密封、隔阻或加固的复合层压板以改善压缩性能的方法,所述方法包括:
提供具有至少35达因/cm的高表面张力的加固层;
将环氧基可膨胀结构泡沫材料置于加固层上形成复合层压板,其中结构泡沫材料和加固层的表面张力在彼此的15达因/cm以内;
其中加固层和结构泡沫材料的高表面张力为负荷从结构泡沫材料转移至加固层提供足够的润湿,以便:
i.与单独的加固层或单独的结构泡沫材料的拉伸强度相比,增加根据ASTMD638的复合层压板的拉伸强度;和
ii.与单独的加固层或单独的结构泡沫材料的搭接剪切强度相比,增加根据ASTMD1002的复合层压板的搭接剪切强度,
其中加固层包括羧酸化学官能团,且结构泡沫材料包括在暴露于高于150℃的温度时与加固层的羧酸形成共价键的组分。
2.权利要求1的方法,包括将复合层压板暴露于高于150℃的温度以便在加固层和结构泡沫材料之间形成共价键的步骤。
3.权利要求1或2的方法,其中加固层包括胺化学官能团,结构泡沫材料包括在暴露于高于150℃的温度时与加固层的胺形成共价键的组分。
4.权利要求1或2的方法,其中加固层包括金属箔。
5.权利要求1或2的方法,其中加固层包括选自以下的聚合膜:丙烯酸酯类树脂、聚酰胺、聚碳酸酯、聚醚胺、聚对苯二甲酸乙二酯、聚酰亚胺、聚砜、聚氯乙烯、酚醛塑料、或其任意结合物。
6.权利要求1或2的方法,其中加固层包括选自以下的膜:缩醛。
7.权利要求1或2的方法,其中加固层的表面进行处理以便提高其表面张力至至少35达因/cm。
8.权利要求7的方法,其中加固层通过涂布液体底漆、电晕放电或用石油基气体和空气混合物燃烧来处理以便提高其表面张力至至少35达因/cm。
9.权利要求1的方法,其中结构泡沫材料包括与加固层的羧酸形成共价键的环氧树脂。
10.权利要求3的方法,其中结构泡沫材料包括与加固层的胺形成共价键的环氧树脂。
11.权利要求1或2的方法,其中结构泡沫材料通过共挤压过程置于加固层上。
12.权利要求11的方法,其中加固层和结构泡沫材料之间的共价键不在共挤压过程期间形成。
13.一种为结构提供密封、隔阻或加固的复合层压板用于改善压缩性能的用途,所述复合层压板包括:
表面张力至少为35达因/cm的加固层;
置于加固层上以形成复合层压板的环氧基可膨胀结构泡沫材料,其中结构泡沫材料和加固层的表面张力在彼此的15达因/cm以内以便改善结构泡沫材料和加固层之间的粘合性,
其中加固层包括羧酸化学官能团,且环氧基可膨胀结构泡沫材料在暴露于高于150℃的温度时与加固层的羧酸形成共价键。
14.权利要求13的用途,其中加固层包括金属箔。
15.权利要求13的用途,其中加固层包括选自以下的聚合膜:丙烯酸类树脂、聚酰胺、聚碳酸酯、聚醚胺、聚对苯二甲酸乙二酯、聚酰亚胺、聚砜、聚氯乙烯、酚醛塑料、或其任意结合物。
16.权利要求13的用途,其中加固层包括选自以下的膜:缩醛。
17.权利要求15或16的用途,其中加固层的表面进行处理以便提高其表面张力至至少35达因/cm。
18.权利要求17的用途,其中加固层通过涂布液体底漆、电晕放电或用石油基气体和空气混合物燃烧来处理以便提高其表面张力至至少35达因/cm。
19.权利要求13或14的用途,其中结构泡沫材料包括:
i.环氧树脂;
ii.环氧/弹性体加合物,所述加合物包括1:3至3:1份的环氧与弹性体;以及
iii.芯/壳聚合物抗冲改性剂。
20.权利要求19的用途,其中加固层包括胺化学官能团,且结构泡沫材料的环氧树脂在暴露于高于150℃的温度时与加固层的胺形成共价键。
21.一种形成为结构提供密封、隔阻或加固的复合层压板以改善压缩性能的方法,所述方法包括:
提供具有至少35达因/cm的表面张力的加固层,其中加固层包括羧酸或胺化学官能团;
通过共挤压过程将环氧基可膨胀结构泡沫材料置于加固层上形成复合层压板,其中结构泡沫材料包括:
i.环氧树脂;
ii.环氧/弹性体加合物,所述加合物包括1:3至3:1份的环氧与弹性体;以及
iii.芯/壳聚合物抗冲改性剂;
其中在暴露于高于150℃的温度时环氧树脂与加固层的羧酸或胺形成共价键;
将复合层压板暴露于高于150℃的温度以便在加固层和结构泡沫材料之间形成共价键;
其中共价键允许负荷从结构泡沫材料转移至加固层,以便与单独的加固层或单独的结构泡沫材料的拉伸强度相比,提高根据ASTMD638的复合层压板的拉伸强度。
22.权利要求21的方法,其中在复合层压板暴露于高于150℃的温度时,加固层和结构泡沫材料之间的共价键基本防止泡沫的横向膨胀以使泡沫的膨胀基本垂直。
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- 2011-03-04 BR BR112012022319A patent/BR112012022319B1/pt not_active IP Right Cessation
- 2011-03-04 US US13/040,704 patent/US9096039B2/en active Active
- 2011-03-04 WO PCT/US2011/027166 patent/WO2011109699A1/en active Application Filing
- 2011-03-04 JP JP2012556261A patent/JP2013521163A/ja not_active Ceased
- 2011-03-04 KR KR1020127025220A patent/KR20130020772A/ko not_active Application Discontinuation
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BR112012022319B1 (pt) | 2020-01-28 |
CN103153604A (zh) | 2013-06-12 |
JP2013521163A (ja) | 2013-06-10 |
WO2011109699A8 (en) | 2013-03-14 |
EP2542403B1 (en) | 2015-05-06 |
US20120028032A1 (en) | 2012-02-02 |
KR20130020772A (ko) | 2013-02-28 |
US9096039B2 (en) | 2015-08-04 |
EP2542403A1 (en) | 2013-01-09 |
BR112012022319A2 (pt) | 2017-10-03 |
WO2011109699A1 (en) | 2011-09-09 |
EP2542403B2 (en) | 2023-08-16 |
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