CN104428132A - 用于自动铺放的复合材料 - Google Patents

用于自动铺放的复合材料 Download PDF

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CN104428132A
CN104428132A CN201380012889.9A CN201380012889A CN104428132A CN 104428132 A CN104428132 A CN 104428132A CN 201380012889 A CN201380012889 A CN 201380012889A CN 104428132 A CN104428132 A CN 104428132A
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composite material
backing paper
flaky composite
composite
flaky
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CN104428132B (zh
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J·埃利斯
E·菲塞
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CEL COMPOSITES Ltd
Hexcel Composites Ltd
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CEL COMPOSITES Ltd
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Abstract

本发明涉及一种片状复合材料，所述片状复合材料包含结构层和可固化热固性树脂，并且在其一个外表面上包含纤维增强背纸。

Description

用于自动铺放的复合材料
技术领域
本发明涉及适于应用于自动铺带设备中的复合材料。
背景技术
复合材料具有文件充分记载的优于传统构造材料的优点，尤其在于以极低的材料密度提供极佳的机械性质。因此，此类材料的使用变得日益普遍，并且其应用领域从“工业”和“运动与休闲”直至延伸到高性能航天部件。
此类复合材料包含结构元件，诸如浸渍有包含树脂诸如热固性或热塑性树脂的组合物的纤维层。
包含浸渍有可固化热固性树脂的纤维布置物的预浸物现在被广泛用于制备此类复合材料。这些使得可小心的控制纤维和树脂的量，并且在它们可以呈现的形状中提供柔韧性。
典型地，可视需要将数个此类预浸物的层“铺放(lay‐up)”，并且典型地通过暴露于升高的温度而使所得的层压物固化，以产生固化的复合层压物。
在历史上是由熟练操作员的手将此类预浸物或类似材料铺放。然而，现代铺放方法包括自动铺放方法、诸如所谓的自动铺带设备(automatictape lay‐up apparatus)或ATL的巨大贡献。
典型的ATL机器需要材料卷，所述材料卷装载到芯轴上，并且经由辊系统馈送到ATL头。典型地，路线包括切割阶段和任选的加热阶段。切割阶段确保材料的尺寸刚好如所需要，因为任何偏差都会导致不可接受的结局。在ATL头处，通常存在两种应用方法，即ATL“套筒”或ATL头的“压紧辊”。无论采用哪种方法，都要使材料与表面接触，并且向隔离纸的最上面的背片上施加压力。最下面的粘性表面在压力下粘着，并且自动地移除背片。在此过程期间，使材料在300mm的典型产品宽度上暴露于50与300N之间的极高张力。
为了使预浸物或类似材料通过自动化机器铺放，其需要根据准确规格来制备。为方便起见，此类材料典型地提供在准备好将材料馈送到ATL设备的卷形物(roll)上。
由于复合材料通常是粘性的，所以复合材料必需具有可剥离的背片，以防止相邻层粘附在卷形物上。此类背片典型地由纸制成。
背片还使得ATL设备可向复合材料施加力，以在铺放期间诱发粘附，其中设备头不粘附到复合材料。
因此，背片典型地仅在ATL设备已经铺设复合材料之后被移除。
在此方法的改进中，可以通过形成ATL设备的一部分的刀片在复合材料中进行切入。此类刀片非常精密，可切穿复合材料并且穿入背纸中一定的短距离(即零点几毫米)。向背层中的部分切入优选地完全切割复合材料，同时维持连续背片，以沿胶带长度拾取张力。操作员将旨在例如切割背层厚度的至多约10％。典型地，使用超声切割器或机械刀片来切割材料。切割ATL胶带具有以下效果：可以引入形状和轮廓，从而给予ATL设备可以处理的铺放设计范围以灵活性。
在典型的方法中，当穿过背片进行切入时，在“压紧辊”处向上提起ATL设备的“套筒”，移动到适当位置，以确保切口一侧的部分复合材料不会被铺设，而是被带走，从而以废弃物形式保持附着于其背片。
一旦铺设好含有切口的部分后，ATL提起压紧辊并同时降低套筒，以继续进行铺设整个复合材料的正常操作。
然而，此类转移通常包括在复合材料上的张力尖峰(spike)。此类力在穿过背纸进行切入期间也扩大。成问题的是，恰好在复合材料已被切割并且削弱时张力尖峰趋于累积，例如在套筒与压紧辊对换时，从而会导致背层断裂。
复合物的切割导致在背片层中的部分切入，但有时这也可以是完全切入，由此背层在胶带有卷曲趋势的边缘处被切割。部分切入具有向背片中引入弱点或应力集中的效果。其结果是背片撕裂且破坏的趋势。背片的撕裂会阻止ATL系统连续馈送更多的ATL胶带，其需要停止自动化过程，同时将破坏的材料移除。这会增加所述过程的成本并且降低其效率。背层的破坏还会导致在一段长度的新胶带必须通过ATL机器以恢复进行连续馈送时废弃物有所增加，另外在断裂之前沉积长度的胶带必须被移除和置换。
另外，背片的断裂可能会导致来自背片的污染碎片被引入到铺放中。
因此，可以解决此问题的任何方式都将是非常合乎需要的。
发明内容
根据本发明，提供一种片状复合材料，所述片状复合材料包含如随附权利要求中任一项中定义的纤维增强的背层。
在第一方面，本发明涉及一种片状复合材料，所述片状复合材料包含结构层和可固化热固性树脂，并且在其一个外表面上包含纤维增强的背纸。
已经发现，通过在背纸中包括纤维增强体，则爆破强度和撕裂抗性得到极大提高，因此在铺设这种材料时，可提高效率、减少ATL过程的时间、废弃物和污染。
尽管此方法解决了一个显著问题，但已经发现向背纸中引入增强纤维会导致纤维的图案转移到复合材料的树脂中。对于一些应用来说，这是不合要求的，需要的是无图案的材料。
此外已经发现，此类图案转移可以通过在纤维增强背纸与复合材料的其余部分之间引入第二背纸而显著减少或完全消除。第二背纸不含有纤维增强体，可保护复合材料的其余部分免于纤维增强体按压到树脂中。
已经发现，如果第二背纸相对不可压缩，那么图案转移可以进一步减少或消除。举例来说，可以使用高度砑光的纸，诸如玻璃纸。另外，整个背层可以在组装期间和在施用到复合材料之前经压缩，由此降低其在施用到复合材料后的可压缩性。
还已发现，对于一些应用来说，纤维图案向树脂表面中的转移可以给空气和挥发物引入排放路径，这可以导致最终层压物的孔隙率有益地降低。因此，在本发明的替代性实施方案中，背片层包含可压缩的第二背纸，诸如牛皮纸。可压缩的第二背纸可以围绕下层纤维变形，由此使相邻树脂图案化。此外，下层纤维的可压缩性、编织图案和直径还可以经调节以改变图案化排放路径的大小和数目。
然而，引入第二背纸还引入可能会带来其它问题如起皱和卷曲的风险。此类问题由于相对膨胀而发生，尤其在储存期间和在变化的湿度环境中。两个层之间的相对膨胀可能会导致纸的卷曲作用或起皱，这两种情况都是非常不合要求的。因此，优选的是可以包括第三背纸以防止此类卷曲或起皱。第三背纸可以适宜地插入到背片内的任何位置，然而它优选地夹在第二与第一背纸之间。
复合材料的结构层可以是能够浸渍有热固性树脂的任何固体材料。
结构层可以包括多孔金属片，诸如扩展箔，或它可以包括纤维的结构层。
适用作扩展箔的金属包括任何导电金属，诸如青铜、铝、铜、银、金、镍、锌和钨。铜由于其极佳导电性而是优选的。结构纤维层中的任何纤维都可以是单向的、织物形式的、无规的或多轴的。在一个优选实施方案中，纤维是单向的。在铺放之后，例如可通过布置使邻近层中的纤维以显示邻近纤维层之间的角度的所谓的0/90布置而正交于彼此，其定向典型地在复合材料如预浸物或半浸渍物的各处变化。在许多其它的布置之中，其它布置如0/+45/‐45/90当然也是可以的。
以上论述的第一、第二和第三纸片和增强纤维中的任一者可以按任何所需次序施用。优选地，第二背纸与结构层相邻，增强纤维和/或第三背纸与第二背纸相邻，最终第一背纸置于第三背纸或纤维增强体任何一个的最上面。
结构纤维可包含破裂的(即拉伸断裂的)选择性不连续或连续的纤维。
结构纤维可以由多种材料制成，诸如玻璃、碳、石墨、镀金属的聚合物芳香族聚酰胺(aramid)和其混合物。复合材料典型地包含30‐70wt％结构纤维。
如上所述，本发明的复合材料包含可固化热固性树脂。可固化树脂可以以离散层形式存在，或可以完全或部分浸渍到结构纤维的层中。复合材料典型地包含15‐50w.t％的可固化树脂，或更优选地32‐45wt.％的可固化树脂。
可固化树脂可以选自本领域中通常已知的那些，诸如酚醛树脂、脲醛树脂、1,3,5‐三嗪‐2,4,6‐三胺(三聚氰胺)、双马来酰亚胺、环氧树脂、乙烯基酯树脂、苯并噁嗪树脂、聚酯、不饱和聚酯、氰酸酯树脂或其混合物。
尤其优选环氧树脂，如单官能、双官能或三官能或四官能环氧树脂。
环氧树脂可以包含单官能、双官能、三官能和/或四官能环氧树脂。
举例来说，适合的双官能环氧树脂包括基于以下的那些：双酚F、双酚A的二缩水甘油醚(任选地溴化)、苯酚和甲酚环氧树脂线性酚醛树脂、酚醛加合物的缩水甘油醚、脂肪族二醇的缩水甘油醚、二缩水甘油醚、二甘醇二缩水甘油醚、芳香族环氧树脂、脂肪族聚缩水甘油醚、环氧化烯烃、溴化树脂、芳香族缩水甘油胺、杂环缩水甘油亚脒和酰胺、缩水甘油醚、氟化环氧树脂或其任何组合。
双官能环氧树脂可以优选地选自双酚F的二缩水甘油醚、双酚A的二缩水甘油醚、二缩水甘油基二羟基萘或其任何组合。
举例来说，适合的三官能环氧树脂可以包括基于以下的那些：苯酚和甲酚环氧线性酚醛树脂、酚醛加合物的缩水甘油醚、芳香族环氧树脂、脂肪族三缩水甘油醚、二脂肪族三缩水甘油醚、脂肪族聚缩水甘油醚、环氧化烯烃、溴化树脂、三缩水甘油基氨基苯基、芳香族缩水甘油胺、杂环缩水甘油亚脒和酰胺、缩水甘油醚、氟化环氧树脂或其任何组合。
适合的四官能环氧树脂包括N,N,N',N'‐四缩水甘油基‐间二甲苯二胺(可以名称Tetrad‐X商购自Mitsubishi Gas Chemical Company，以及以ErisysGA‐240商购自CVC Chemicals)，和N,N,N',N'‐四缩水甘油基亚甲基二苯胺(例如来自Huntsman Advanced Materials的MY721)。热固性树脂还可以包含一种或多种固化剂。适合的固化剂包括酐，尤其聚羧酸酐；胺，尤其芳香族胺，例如1,3‐二氨基苯、4,4'‐二氨基二苯甲烷；和尤其砜，例如4,4'‐二氨基二苯砜(4,4'DDS)和3,3'‐二氨基二苯砜(3,3'DDS)；和酚醛树脂。优选的固化剂是氨基砜，尤其4,4'DDS和3,3'DDS。
树脂和纤维的类型和设计的其它实例可以见于WO 2008/056123中。
背片中的纤维增强可以呈多种形式，例如它们可以是编织、针织、无规或水刺的。优选纤维是编织的，因为其提供良好的强度而无过多的突出物被引入到背纸，编织织物可确保纤维具有规则布置。已经发现这样可使得背片中的撕裂扩散大大减少。此外，优选的是背片中的纤维增强体由连续纤维制成，因此当切割纤维时，其牢固锚定于背片内。在不连续纤维的无规垫或片的情况下，可能会在切割时产生小片段，这可能会污染铺放物。
在一个实施方案中，背层的纤维增强体可以包含热塑性纤维，如聚乙烯、聚醚砜、尼龙、凯芙拉、本领域所熟知的其它热塑性纤维、玻璃、碳、石墨、玄武岩或其它合成纤维和天然纤维，包括亚麻、黄麻、棉布等。在优选的实施方案中，纤维增强体包含聚乙烯。优选地，纤维被编织到织物中，在优选的实施方案中，它被编织到3向格栅中。
在一个实施方案中，纤维增强体被编织到具有经纱和纬纱方向的纤维的织物中。在一个实施方案中，经纱纤维可以与结构层胶带的纵向方向实质上平行地对准。或者，经纱可以与纵向方向成一定角度、例如+/‐45°布置。
优选地，纤维增强体是面积重量为4‐100gsm或更优选地10‐60gsm或更优选地5‐30gsm或更优选地12‐24gsm或更优选地17‐19gsm的层。
优选地，第一背纸包含聚合物片或纤维素纸。第一背片优选地包含有机硅涂层，以便当卷绕到卷形物上时防止背层的最外表面粘附到结构层。优选地，背层的面积重量是25‐100gsm或更优选地34‐66gsm或更优选地44‐56gsm或更优选地48‐52gsm。
优选地，第二背纸包含聚合物片或更优选地纤维素纸。第二背片优选地包含有机硅涂层以减少结构层与背片之间的粘着力，使得两者在ATL布置期间可分离。优选地，背层的面积重量是25‐100gsm或更优选地34‐66gsm或更优选地44‐56gsm或更优选地48‐52gsm。
第三背片可以包含适用于第一或第二背纸的任何材料。优选地，第三背片包含聚合物片，诸如聚酰胺、聚醚‐对苯二甲酸酯、聚醚砜、丙烯酸酯聚合物、聚酯或其共聚物。最优选地，聚合物片包含聚乙烯。
优选地，第三背纸的面积重量是5‐100gsm或更优选地10‐50gsm或更优选地20‐34gsm或更优选地23‐27gsm。
当使用NFQ03019或ASTM D646测量时，包含第一、第二或第三背纸和纤维增强体任何之一的背片优选地组合厚度是50‐500μm，或更优选地100‐400μm或更优选地150‐300μm或更优选地75‐225μm。
优选地，当根据ASTM D828评估时，背片展现出至少5daN/15mm或更优选地10daN/15mm或更优选地至少15daN/15mm的机器方向的机械阻力。优选地，当使用ASTM D828评估时，背片在垂直于机器方向的方向上具有至少3daN/15mm或更优选地至少5daN/15mm或更优选地至少9daN/15mm的机械阻力。
优选地，当根据TAPPI T470评估时，背片展现出至少1.0daN/15mm或更优选地至少2.0daN/15mm或更优选地至少3.0daN/15mm的机器方向的撕裂抗性。优选地，当使用TAPPI T470评估时，背片在垂直于机器方向的方向上展现出至少1daN/15mm或更优选地2.0daN/15mm或更优选地2.5daN/15mm的撕裂抗性。
优选地，当使用ASTM D774评估时，背片展现出至少200KPa或更优选地400KPa的爆破强度。优选地，背片展现出大于50g/m2/24h或更优选地大于100g/m2/24h的水蒸气传输速率。
机器方向是ATL胶带的长度方向，即平行于ATL系统所用的加工方向的方向。
本发明的复合材料可以视需要包括额外材料，诸如性能增强剂或改性剂。此类材料可以选自柔化剂、增韧剂/颗粒、额外促进剂、核壳橡胶、阻燃剂、熔化剂、颜料/染料、增塑剂、UV吸收剂、抗真菌组分、填充剂、粘度调节剂/流动控制剂、稳定剂和抑制剂。
然而，优选地，复合材料的厚度是0.5‐5.0mm、更优选地0.5‐4.0mm、最优选地1.0‐3.0mm，以便它适宜地可以由ATL设备处理。
由于复合材料计划以卷形物形式提供，因此优选其足够柔软，以便能够当背片施用到复合材料时形成最小直径小于20cm、优选小于10cm或更优选小于250mm或当它施用到树脂膜时小于70mm的卷形物。
根据本发明的复合材料可以通过本领域中已知的任何方法来制备。此类方法典型地包括使结构层与热固性树脂结合在一起，和用树脂浸渍结构层。一旦制备后，通常将复合材料卷起来，以备由ATL设备沉积。
因此，在第二方面，本发明涉及一种将如本文中所述的复合材料铺设到衬底上的方法，将所述复合材料从卷形物自动馈送到所述衬底，以便背纸在最上面，所述复合材料通过用工具向所述背纸上施加压力而粘附到所述衬底，随后移除所述背纸，使复合材料就位在所述衬底上而无其背纸。
在优选的实施方案中，所述方法包括切穿结构层并且部分切割到背纸层中，随后铺设复合材料。
在此情况下，重要的是切割器不切割到背纸中太深而还切割增强纱线，否则背纸的撕裂性质会大大降低。
此方法典型地接下来是后续安置额外的复合材料如预浸物，以产生复合材料的堆叠物。
一旦复合材料被铺设后，布置通过暴露于升高的温度和任选存在的升高的压力而固化，以产生固化的复合材料。
附图说明
现在将仅以实例的方式并且参考以下图式来说明本发明，其中：
图1是用于本发明中的增强背纸的示意图。
图2是用于本发明中的另一增强背纸的示意图。
图3是穿过根据本发明的复合材料的截面图。
图4是穿过根据本发明的另一复合材料的截面图。
图5是用于根据本发明的过程中的ATL设备的侧视图。
图6是根据本发明的、在铺放期间已经因在切割之后撕裂而破坏的背纸的示意图。
图7是复合材料在图6中所示的撕裂之前的切割期间的截面图。
图8是复合材料在不导致如图6中所示的撕裂的切割期间的截面图。
具体实施方式
就附图而言，图1展示用编织棉纱线12增强的背纸片10。棉纱线以规则编织物形式编织，并且经纱和纬纱分别在0°和90°方向上对准。
图2展示用具有不同图案的编织纱线增强的另一背纸片14。
图3展示根据本发明的复合材料20。复合材料20包含预浸物层22，所述预浸物层包含浸渍有可热固化环氧树脂的单向纤维结构层(未展示)。两层的背纸附着于此，所述背纸包含用编织棉纱线26增强的背纸24，和不含编织纱线且被超级砑光、以便其具有极低的可压缩性的第二背纸28。
图4展示根据本发明的另一种复合材料30。复合材料30包含预浸物层32，所述预浸物层包含浸渍有可热固化环氧树脂的单向纤维结构层(未展示)。三层的背纸附着于此，所述背纸包含用编织棉纱线37增强的背纸34，不含编织纱线且被超级砑光、以便它具有极低的可压缩性的第二背纸38，和第三背纸39。
图5展示铺设根据本发明的复合材料的ATL设备的侧视图。复合材料40从具有中心核42的卷材料馈送通过切割台44到ATL头46。在铺放之后，预浸物48优先粘附到衬底50，将背纸52移除到收取辊54上。
在正常操作中，不对预浸物进行切割，并通过将所述头46按压到复合材料上进行铺放。
当需要切割时，则将头46向上提起，并且将压紧辊47向下移动，以与已铺设的预浸物48接触。这具有如下效果，预浸物的切割掉的部分不被铺设，但保持附着于背纸，并且由收取辊54拾取。头与辊的对换会在复合材料中引入张力峰值，这可能会引发背纸撕裂。
一旦切割停止后，就将压紧辊47提起而不与预浸物48接触，并且头46再次向下移动，以通过向背纸52上施加压力而连续铺放。
切割台44包括两个超声切割装置56、58，它们可以被程序化以切穿预浸物48，并部分切割到背纸52中。切割器56、58被程序化，以穿入背纸厚度的10％，以便确保完全切穿预浸物而不过分弱化背纸。另外，必须小心不切穿增强纱线，因为这将会移除它们已经提供的任何撕裂强度。
图6展示根据本发明使用的增强纸背片60。然而，如图7中所示，切割器56已经被设置为太深地切穿背纸，并且已经切穿增强纱线26。这产生了撕裂62，导致铺放过程停止，同时材料被重配置。
图8展示用于切割器58的正确设置，其中切割器58不切穿纱线26。此背纸当用于ATL过程中时即使在切割期间也不会被破坏。本发明现在将通过参考以下实施例而明朗化。
实施例
组装背片，所述背片按以下次序包含以下层：
第一背纸：50g/m2的高砑光玻璃纸
第三背纸：24g/m2的聚乙烯片
纤维增强体：18g/m2的编织的双向的聚乙烯格栅
第二背纸：50g/m2的高砑光玻璃纸
通过使用轧辊(nip roller)进行压制来组装背片，随后将有机硅涂层涂敷到外表面。背片进行机械测试，其结果列在表1中：
表1.机械测试的结果
使背片的第二背纸与M21/EV预浸物(Hexcel Composites Ltd.DuxfordUK)层接触，并且使用轧辊巩固，然后将其切开，并且卷动以形成ATL匹配胶带(compatible tape)。
将ATL胶带装载到ATL系统中，并且沉积到模具表面上。预浸物和背层展现出与模具表面的良好粘性，以及与后续预浸物层的良好粘性。将胶带使用集成到ATL系统中的切割设备与胶带方向成90°地切割，预浸物经整齐切割，并且背层保持未被切割，并且适用于ATL胶带的连续馈送，因此展现背片与ATL铺放的匹配性。

Claims (16)

1.一种片状复合材料，所述片状复合材料包含结构层和可固化热固性树脂，并且在其一个外表面上包含纤维增强背纸。
2.根据权利要求1所述的片状复合材料，所述片状复合材料在所述纤维增强背纸与所述复合材料的其余部分之间包含第二背纸。
3.根据权利要求2所述的片状复合材料，其中所述第二背纸的可压缩性小于0.001kg‐1m‐2。
4.根据以上权利要求中任一项所述的片状复合材料，其中所述结构层包含金属扩展箔。
5.根据以上权利要求中任一项所述的片状复合材料，其中所述结构层包含纤维的结构层。
6.根据权利要求5所述的片状复合材料，其中所述纤维是单向的。
7.根据权利要求5或权利要求6所述的片状复合材料，所述片状复合材料包含30‐70wt％的结构纤维。
8.根据以上权利要求中任一项所述的片状复合材料，其中背片中的纤维增强体是织造的。
9.根据以上权利要求中任一项所述的片状复合材料，所述片状复合材料的厚度是0.5‐5.0mm，优选0.5‐4.0mm，更优选1.0‐3.0mm。
10.根据以上权利要求中任一项所述的片状复合材料，所述片状复合材料足够柔软，以便能够形成直径小于20cm、优选小于10cm的卷形物。
11.一种将根据以上权利要求中任一项所述的片状复合材料铺设到衬底上的方法，将所述片状复合材料从卷形物自动馈送到所述衬底，以便背纸在最上面，并且所述复合材料通过用工具向所述背纸上施加压力而粘附到所述衬底，随后移除所述背纸，使所述复合材料就位在所述衬底上而无其背纸。
12.根据权利要求11所述的方法，所述方法在铺设所述复合材料之前包括以下步骤：切穿结构层，且部分地切割到所述背纸层中。
13.根据权利要求12所述的方法，其中所述切割不切穿所述背纸中的增强纱线。
14.根据权利要求11到13中任一项所述的方法，所述方法之后是后续安置额外的复合材料，以产生复合材料的堆叠物。
15.根据权利要求11到14中任一项所述的方法，所述方法之后是通过暴露于升高的温度和任选存在的升高的压力而固化，以产生固化的复合材料。
16.一种固化的复合材料，其可通过根据权利要求15所述的方法获得。
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