CN102947076B - 包含连续纤维和长纤维的热塑性预浸料坯 - Google Patents

包含连续纤维和长纤维的热塑性预浸料坯 Download PDF

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Publication number
CN102947076B
CN102947076B CN201180029246.6A CN201180029246A CN102947076B CN 102947076 B CN102947076 B CN 102947076B CN 201180029246 A CN201180029246 A CN 201180029246A CN 102947076 B CN102947076 B CN 102947076B
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China
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prepreg
continuous fiber
long fibre
thermoplasticity
fibre
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CN201180029246.6A
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CN102947076A (zh
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J·J·玛丽泽维斯基
A·H·约翰逊
T·L·迪波尔
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Ticona LLC
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Ticona LLC
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    • B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
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    • B29C70/00—Shaping composites, i.e. plastics material comprising reinforcements, fillers or preformed parts, e.g. inserts
    • B29C70/04—Shaping composites, i.e. plastics material comprising reinforcements, fillers or preformed parts, e.g. inserts comprising reinforcements only, e.g. self-reinforcing plastics
    • B29C70/06—Fibrous reinforcements only
    • B29C70/08—Fibrous reinforcements only comprising combinations of different forms of fibrous reinforcements incorporated in matrix material, forming one or more layers, and with or without non-reinforced layers
    • B29C70/081—Combinations of fibres of continuous or substantial length and short fibres
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Abstract

提供了包含嵌入在热塑性聚合物基体(127)内的多个单向排列的连续纤维(142)的预浸料坯。除连续纤维之外，该预浸料坯还包含多个长纤维，使得它们在热塑性基体内无规分布。因此，至少一部分该长纤维变得相对于该连续纤维的方向成一定角度取向。该长纤维能够显著增加预浸料坯在横向方向的机械性能。

Description

包含连续纤维和长纤维的热塑性预浸料坯
相关申请
本申请要求2010年6月22日提交的临时申请序列号61/357,301的优先权，其全部内容通过引用并入本文。
背景技术
增强复合材料（或“预浸料坯”）通常是由浸渍在树脂基体内的纤维（例如碳纤维或玻璃纤维）制成。热固性树脂（例如不饱和聚酯、环氧树脂或聚酰亚胺）通常用作基体，特别是在需要高强度水平的应用中。然而，由热固性树脂制成的预浸料坯的一个问题是其通常脆性且具有差的抗冲击性。此外，由于该树脂的保存期限短，因此该预浸料坯通常难以储存。在为了克服这些问题的尝试中，近来努力开发热塑性预浸料坯。一种这样的预浸料坯是由热塑性树脂和单向排列的连续纤维制成的。这样的预浸料坯在纤维轴方向的弹性模量和强度方面具有优良的性能。然而，由于这样的预浸料坯具有各向异性的机械性能，因此在使用中需要在不同方向上取向的多个预浸料坯层。这必然引起所得到部件的成本的提高和厚度的增加。为解决与热固性预浸料坯相关问题的其它尝试包括使用热塑性树脂和通过切割单向排列的纤维束形成的短纤维。尽管这样的预浸料坯呈现出较好的各向同性强度性能，但增强纤维的最大体积分数通常低，这导致相对差的弹性模量和强度。此外，难以通过控制这种短纤维的体积来调节预浸料坯的机械性能。
如此，目前存在对根据具体应用选择性地控制其机械性能的热塑性预浸料坯的制备方法的需要。还存在对具有各向同性的机械性能的热塑性预浸料坯的需要。
发明内容
依照本发明的一个实施方案，公开了包含基本上在纵向方向上取向的多个连续纤维和无规分布的多个长纤维的热塑性预浸料坯，至少一部分长纤维以相对于该纵向方向成一定角度取向。连续纤维构成预浸料坯的约10wt%-约80wt%，长纤维构成预浸料坯的约2wt%-约35wt%。预浸料坯还包含树脂基体，其包含一种或多种热塑性聚合物且连续纤维和长纤维嵌入在其中，其中热塑性聚合物构成预浸料坯的约10wt%-约80wt%。预浸料坯在纵向方向的最大拉伸应力与预浸料坯在横向方向的最大拉伸应力的比值为约1-约40。
依照本发明的另一实施方案，公开了热塑性预浸料坯的制备方法。该方法包括将连续纤维和长纤维供给挤出装置，并将热塑性进料供给挤出装置，其中该进料包含至少一种热塑性聚合物。将连续纤维、长纤维和热塑性聚合物在浸渍模具内挤出以形成其中连续纤维与长纤维混杂并用热塑性聚合物基体嵌入的挤出物。
依照本发明的另一实施方案，公开了热塑性预浸料坯的制备方法。该方法包括将连续纤维和热塑性进料供给挤出装置，其中该进料包含至少一种热塑性聚合物。将连续纤维和进料在浸渍模具中挤出以形成其中连续纤维嵌入有热塑性聚合物基体的挤出物。然后将长纤维施加到挤出物中以形成复合材料。
下面更详细地提出了本发明的其它特征和方面。
附图简述
在说明书的剩余部分中，包括参照附图，更具体地提出了本发明的完整和能够实现的公开内容，包括对本领域技术人员而言的其最佳方式，在附图中：
附图1是用于本发明中的浸渍系统的一种实施方案的示意图；
附图2A是图1中所示的浸渍模具的截面视图；
附图2B是可在本发明中使用的浸渍模具的歧管组件和浇道的一种实施方案的部件分解图；
附图2C是至少部分地限定可在本发明中使用的浸渍区域的板的一种实施方案的透视图；
附图3是用图1的系统制备的预浸料坯的一种实施方案的横向截面视图；
附图4是图3中所示的预浸料坯的纵向截面视图；
附图5是可在由本发明的预浸料坯制备型材中使用的拉挤系统的一种实施方案的示意图；
附图6是本发明制备的预浸料坯的阳极实施方案的横向截面视图；
附图7是图6中所示预浸料坯的纵向截面视图；
附图8是在制备本发明的预浸料坯中使用的浸渍系统的仍另一实施方案的示意图；
附图9是用图8的系统制备的预浸料坯的一个实施方案的横向截面视图；
附图10是图9中所示的预浸料坯的纵向截面视图；和
附图11是可依照本发明制备的型材的一个实施方案的截面视图。
在本说明书和附图中参考标记的重复使用意于表示本发明的相同或类似的特征或要素。
具体实施方式
本领域普通技术人员应当认识到目前的讨论仅是对示例性实施方案的描述，并不意于为限制本发明的较宽方面。
一般而言，本发明涉及包含嵌入在热塑性聚合物基体内的多个单向排列的连续纤维的预浸料坯。除连续纤维之外，该预浸料坯还包含与连续纤维结合的多个长纤维，使得它们在热塑性基体内无规分布。因此，至少一部分该长纤维变得相对于该连续纤维的方向成一定角度（例如垂直）取向。通过这样的定位，该长纤维能够显著增加预浸料坯在横向方向的机械性能（例如强度）并因此达到更各向同性的材料。尽管独特的各向同性的预浸料坯是本发明的一个方面，但应当认识到这不是必需的。事实上，本发明的一个显著特征是通过选择性地控制某些工艺参数例如使用的长纤维的类型、使用的连续纤维的类型、长纤维的浓度、连续纤维的浓度、使用的热塑性树脂等从而能够调节用于意欲应用的预浸料坯的机械性能。
现在将更详细地描述本发明的各种实施方案。
I.连续纤维
术语“连续纤维”指具有通常仅由部件的长度限制的长度的纤维、细丝、纱线或粗纱(例如纤维束)。例如，这样的纤维可以具有大于约25毫米的长度，在一些实施方案中约50毫米或更长，和在一些实施方案中约100毫米或更长。连续纤维可以由本领域中已知的任意常规材料制成，例如金属纤维、玻璃纤维(例如E-玻璃、A-玻璃、C-玻璃、D-玻璃、AR-玻璃、R-玻璃、S1-玻璃、S2-玻璃)、碳纤维(例如石墨)、硼纤维、陶瓷纤维(例如氧化铝或二氧化硅）、芳族聚酰胺纤维(例如E.I.duPontdeNemours,Wilmington,DE销售的)、合成有机纤维(例如聚酰胺、聚乙烯、聚对苯撑(paraphenylene)、对苯二甲酰胺、聚对苯二甲酸乙二醇酯和聚苯硫醚)和已知用于增强热塑性组合物的各种其它天然或合成的无机或有机纤维材料。玻璃纤维和碳纤维特别理想地于连续纤维中。这样的纤维通常具有约4-约35微米的标称直径，在一些实施方案中为约9-约35微米。纤维可以是绞合的或直的。如果需要，纤维可以是含单一的纤维类型或不同的纤维类型的粗纱(例如纤维束)的形式。不同的纤维可以包含在单个粗纱中，或者替代地，各粗纱可以包含不同的纤维类型。例如，在一个实施方案中，某些粗纱可以包含连续碳纤维，而其它粗纱可以包含玻璃纤维。各粗纱中包含的纤维数目可以是相同的或粗纱之间不同。典型地，粗纱可以包含约1,000纤维-约50,000单纤维，和在一些实施方案中约2,000-约40,000纤维。
II.长纤维
术语“长纤维”通常指不连续的且具有约0.5-约25毫米（在一些实施方案中约0.8-约15毫米，和在一些实施方案中约1-约12毫米)的长度的纤维、细丝、纱线或粗纱。长纤维可以由如上面关于连续纤维所述的任意材料、形状和/或尺寸形成。玻璃纤维和碳纤维特别理想地用作长纤维。
III.热塑性基体
可以使用任意多种热塑性聚合物形成其中嵌入连续纤维和长纤维的热塑性基体。在本发明中使用的适合的热塑性聚合物可以包括例如：聚烯烃（例如聚丙烯、丙烯-乙烯共聚物等）、聚酯（例如聚对苯二甲酸丁二醇酯（“PBT”））、聚碳酸酯、聚酰胺（例如NylonTM）、聚醚酮（例如聚醚醚酮（“PEEK”））、聚醚酰亚胺、聚亚芳基酮(例如聚亚苯基二酮(“PPDK”))、液晶聚合物、聚芳硫醚（例如聚苯硫醚（“PPS”））、含氟聚合物（例如聚四氟乙烯-全氟甲基乙烯基醚聚合物、全氟-烷氧基烷烃聚合物、四氟乙烯聚合物、乙烯-四氟乙烯聚合物等）、聚缩醛、聚氨酯、聚碳酸酯、苯乙烯类聚合物（例如丙烯腈丁二烯苯乙烯（“ABS”））等。ABS是特别适合的热塑性聚合物。
在预浸料坯中可以使用一种或多种热塑性基体。例如，在一个实施方案中，首先例如以下面将描述的方式用第一热塑性基体预浸渍长纤维，然后冷却并切成具有约25毫米或更小长度的颗粒。然后当它们用第二热塑性基体浸渍时，可以将这些颗粒与连续纤维组合。因此，在这个实施方案中，长纤维实际上嵌入在两种热塑性基体内。用于长纤维的第一热塑性基体可以与第二热塑性基体相同或不同。替代地，用于预浸渍长纤维的第一热塑性塑料基体可以组成预浸料坯中存在的唯一热塑性基体。仍在另一实施方案中，不预浸渍长纤维，而是当用热塑性基体浸渍长纤维和连续纤维时，简单地将两者组合。
IV.预浸料坯的制备
如上所述，预浸料坯通常是以能够无规地分布长纤维的方式形成。这可以以多种方式完成。在一个特别的实施方案中，例如，可以将长纤维热塑性颗粒供给到挤出装置的料斗，然后与连续纤维熔融混合。挤出工艺的压力和力引起长纤维在所得到的预浸料坯内的所需的无规取向。参照图1，例如，显示这样的挤出设备的一个实施方案。更具体地，该设备包括含安装在桶122内部的螺杆轴124的挤出机120。加热器130（例如电阻加热器）安装在桶122的外部。在使用中，将热塑性聚合物进料127通过料斗126供给到挤出机120。在该特别的实施方案中，进料127也包含长纤维。长纤维例如构成进料的约5wt%-约60wt%（在一些实施方案中约10wt%-约50wt%，和在一些实施方案中约20wt%-约40wt%）。替代地，进料127可以不含长纤维，这样的纤维可以在另一位置(未示出)供给，例如从料斗126的下游和/或其它进料端。
无论如何，将热塑性进料127在桶122内通过螺杆轴124传送，并通过桶122内的摩擦力和加热器130加热。一经加热，进料127通过桶法兰128离开桶122并进入浸渍模具150的模具法兰132。将连续纤维粗纱142或多个连续纤维粗纱142从一个或多个卷轴144供给到模具150。粗纱142通常在浸渍之前保持分开一定距离，例如至少约4毫米，在一些实施方案中至少约5毫米。进料127可以进一步在模具内部通过安装在模具150内或模具150周围的加热器133加热。模具通常在以足以造成热塑性聚合物熔融和浸渍的温度操作。典型地，模具的操作温度高于热塑性聚合物的熔点，例如在约200℃-约450℃的温度。在以这种方式加工时，连续纤维粗纱142开始嵌入在可以是处理进料127得到的树脂214（图2A）的聚合物基体中，并与其中包含的长纤维混杂。然后将该混合物通过浸渍模具150挤出以产生挤出物152。
压力传感器137（图2A）感应浸渍模具150附近的压力，以通过控制螺杆轴124的转动速度或进料器的进料速率从而允许对挤出速率实施控制。即，压力传感器137位于浸渍模具150的附近使得能够操作挤出机120以输送适当量的树脂214用于与纤维粗纱142的相互作用。在离开浸渍模具150之后，挤出物152或浸渍的纤维粗纱142可进入任选的预成型或导向部分（未示出），然后进入两个相邻辊筒190之间形成的辊隙。虽然是任选的，但辊筒190可有助于将挤出物152合并(consolidate)为条带(带子)形式以及增强纤维浸渍并挤出任何过多的空隙。除了辊筒190之外，也可以使用其它成型装置，例如模具系统。通过安装在辊筒上的履带162和164牵引所得到的合并带156。履带162和164还牵引挤出物152远离浸渍模具150和通过辊筒190。如果需要，可以将合并带156在部分171处缠绕起来。一般而言，条带较薄且典型地具有约0.05-约1毫米的厚度，在一些实施方案中约0.1-约0.8毫米，和在一些实施方案中约0.2-约0.4毫米。
在浸渍模具内，粗纱142横向通过浸渍区域250以用聚合物树脂214浸渍粗纱通常是所需的。在浸渍区域250内，通过浸渍区域250中产生的剪切和压力可推动聚合物树脂通常横向通过粗纱，这显著提高了浸渍的程度。在由高纤维含量（例如约35%重量分数（“Wf”）或更高，和在一些实施方案中约40%Wf或更高）的条带形成复合材料时，这是特别有用的。典型地，模具150将包含多个接触表面252，例如至少2个、至少3个、4-7个、2-20个、2-30个、2-40个、2-50个或更多个接触表面252，以在粗纱142上产生足够的渗透程度和压力。尽管它们的具体形式可能改变，但接触表面252典型地具有曲线表面，例如弯曲的叶片、杆等。接触表面252通常也由金属材料制备。
图2A显示了浸渍模具150的截面视图。如所示，浸渍模具150包含歧管组件220、浇道270和浸渍区域250。提供歧管组件220以使聚合物树脂214流动通过其。例如，歧管组件220可以包含一个或多个通道222。提供给浸渍模具150的树脂214可以流动通过通道222。
如图2B中所示，通道222的一些部分可以是曲线的，在示例性实施方案中，通道222沿中央轴224具有对称的取向。此外，在一些实施方案中，通道可以是多个分岔浇口222，其可以包含第一分岔浇口组232、第二组234、第三组236和如果需要的更多的分岔浇口组。每组可以包括从前一组的流道222或最初的通道222分叉出的2、3、4或更多个流道222。
分岔浇口222和其对称取向通常均匀地分布树脂214，使得离开歧管组件220和涂覆粗纱142的树脂214的流动基本上均匀地分布在粗纱142上。这适宜地允许可以通常均匀地浸渍粗纱142。
此外，在一些实施方案中，歧管组件220可以限定出口区域242，其通常包含树脂214由从其离开的通道或流道222的至少下游部分。在一些实施方案中，位于出口区域242中的至少部分通道或流道222沿着树脂214的流动方向244具有增加的面积。当树脂214流动经过歧管组件220时，该增加的面积允许树脂214的扩散和进一步分布，这进一步允许树脂214在粗纱142上基本上均匀地分布。
如图2A和2B中进一步所示，在流动通过歧管组件220之后，树脂214可以流动通过浇道270。浇道270位于歧管组件220和浸渍区域250之间，且提供用于使来自歧管组件220的树脂214流动使得树脂214涂覆粗纱142。因此，如图所示，离开歧管组件220（例如通过出口区域242）的树脂214可以进入浇道270并从其流过。
一旦如图2A中所示离开模具150的歧管组件220和浇道270，树脂214与横向通过模具150的粗纱142接触。如上所述，由于树脂214在歧管组件220和浇道270中的分布，树脂214可以基本上均匀地涂覆粗纱142。此外，在一些实施方案中，树脂214可以撞击在各粗纱142的上表面上或各粗纱142的下表面上或同时在各粗纱142的上下表面上。对粗纱142的初始撞击提供粗纱142与树脂214的进一步浸渍。
如图2A中所示，涂覆的粗纱142以运行方向282横向通过被构造用树脂214浸渍粗纱142的浸渍区域250。例如，如图2A和2C中所示，粗纱142横向越过浸渍区域中的接触表面252。粗纱142在接触表面252上的撞击产生足以用树脂214浸渍粗纱142的剪切和压力以涂覆粗纱142。
在一些实施方案中，如图2A中所示，浸渍区域250限定在两个间隔开的对置板256和258之间。第一板256限定第一内表面257，而第二板258限定了第二内表面259。接触表面252可以同时限定在第一和第二内表面257和259上或由其延伸，或限定在第一和第二内表面257和259中仅一个上。图2C说明了第二板258和依照这些实施方案形成浸渍区域250的至少一部分的其上的各种接触表面。在示例性实施方案中，如图2A中所示，接触表面252可以交替限定在第一和第二表面257和259上使得粗纱交替地撞击在第一和第二表面257和259上的接触表面252上。因此，粗纱142可以以波浪形式、曲折形式或正弦曲线形状的路径通过接触表面252，这增强了剪切。
粗纱142横向通过接触表面252的角度254通常可足够高以提高剪切，但不能太高以引起将破坏纤维的过大的力。因此，例如，角度254可以在约1°-约30°，和在一些实施方案中约5°-约25°。
在替代的实施方案中，浸渍区域250可以包括多个销(未示出)，各销具有接触表面252。销可以是静态的、自由转动的或转动驱动的。在另一替代的实施方案中，接触表面252和浸渍区域250可以如所需要包含任意适合的形状和/或结构用以用树脂214浸渍粗纱142。
为了进一步促进粗纱142的浸渍，当其在浸渍模具内存在时，也可以将它们保持在张力下。该张力可以例如在每粗纱142或纤维束约5-约300牛，在一些实施方案中约50-约250牛，和在一些实施方案中约100-约200牛的范围内。
如图2A中所示，在一些实施方案中，到达区域280可以位于粗纱142的运行方向282上浸渍区域250的下游。粗纱142可以横向通过到达区域280然后离开模具150。如图2A中进一步所示，在一些实施方案中，面板290可以邻接浸渍区域250。通常构造面板290以计量自粗纱142的过多的树脂214。因此，可以调节粗纱142横向通过其的面板290上的孔使得当粗纱142横向通过其时开孔的尺寸使得从粗纱142上除去过多的树脂214。
但是上面所示和所述的浸渍模具仅是在本发明中使用的多种可能构造的一种。在替代的实施方案中，例如，可以将纤维引入相对于聚合物熔体的流动方向成一定角度定位的十字头模具中。当纤维移动通过十字头模具并到达其中聚合物从挤出机桶中离开的点时，促使聚合物与纤维接触。还应当认识到也可以使用任何其它挤出机设计（例如双螺杆挤出机）。仍进一步，也可任选地使用其它组件以辅助纤维的浸渍。例如，在某些实施方案中可使用“气体喷射”组件以帮助各自可包含高达24,000那么多个纤维的单一纤维的束或捆在组合的捆的整个宽度上的均匀散布。这有助于实现条带中强度性能的均匀分布。这样的组件可以包括压缩空气或其它气体的供给，其以通常垂直的方式撞击在穿过出口端的移动的纤维束上。然后可以将散布的纤维束引入模具中用以浸渍，例如如上所述。
无论使用何种技术，预浸料坯中的至少一部分长纤维以相对于连续纤维取向的纵向方向(图1中系统的机器方向“A”)成一定角度取向。例如，约10%或更多(在一些实施方案中约20%或更多，和在一些实施方案中约30%或更多)的纤维可以以相对于连续纤维的纵向方向成一定角度取向。该角度可以例如为约10°-约120°，在一些实施方案中约20°-约110°，和在一种实施方案中约90°。参照图3-4例如，显示了预浸料坯200的一种实施方案，其包含以相对于其中连续纤维240排列的纵向方向“L”成各种角度取向的多个长纤维220。在其它因素中，取向角度有助于控制预浸料坯的横向强度。
此外，预浸料坯中长纤维和连续纤维的相对百分比也有助于控制强度性能。为了达到拉伸强度和横向强度之间良好的平衡，连续纤维的重量与长纤维的重量之比典型地控制在约0.2-约10，在一些实施方案中约0.4-约5，和在一些实施方案中约0.5-约5。例如，连续纤维可以构成预浸料坯的约10wt%-约80wt%，在一些实施方案中约20wt%-约70wt%，在一些实施方案中约40wt%-约60wt%。同样地，长纤维可以构成预浸料坯的约2wt%-约35wt%，在一些实施方案中约5wt%-约30wt%，和在一些实施方案中约10wt%-约25wt%。热塑性聚合物可以构成预浸料坯的约10wt%-约80wt%，和在一些实施方案中约20wt%-约70wt%，在一些实施方案中约40wt%-约60wt%。
预浸料坯还具有非常低的空隙率，这有助于提高预浸料坯的机械性能。例如，空隙率可以为约3%或更低，在一些实施方案中约2%或更低，和在一些实施方案中约1%或更低。空隙率可以使用对本领域技术人员公知的技术测量。例如，空隙率可以使用“树脂烧尽”试验测定，其中将样品放在烘箱（例如600℃持续3小时）烧尽树脂。然后可以测量剩余纤维的质量以计算重量和体积分数。这种“烧尽”试验可以依照ASTMD2584-08进行，以测定纤维和热塑性基体的重量，然后可以基于以下方程式将其用于计算“空隙率”：
Vf＝100*(ρt-ρc)/ρt
其中：
Vf是作为百分比的空隙率；
ρc是使用已知技术（例如用液体或气体比重瓶（例如氦气比重瓶））测量的复合材料的密度；
ρt是由以下方程式确定的复合材料的理论密度：
ρt=1/[Wf/ρf+Wm/ρm]
ρm是热塑性基体的密度（例如在适当结晶度时的密度）；
ρf是纤维的密度；
Wf是纤维的重量分数；和
Wm是热塑性基体的重量分数。
替代地，空隙率可以依照ASTMD3171-09通过化学地溶解树脂而测定。“烧尽”和“溶解”方法特别适合于玻璃纤维，其通常抗熔融和化学溶解。然而，在其它情况下，可以依照ASTMD2734-09（方法A）基于热塑性聚合物、纤维和条带的密度间接地计算空隙率，其中密度可以依照ASTMD792-08方法A确定。当然，也能够使用常规显微设备估算空隙率。
通过对上述提及的各种参数的控制，可以调节机械强度性能以适应所需的应用。例如，在某些实施方案中，预浸料坯呈现出各向同性的强度性能是所需的。更特别地，对于这样的各向同性的预浸料坯，纵向方向的最大拉伸应力（或“极限强度”）与横向方向的最大拉伸应力之比典型地为约1-约40，在一些实施方案中约2-约30，和在一些实施方案中约4-约20。在某些实施方案中，本发明的预浸料坯可以呈现约250-约3000兆帕（MPa）（在一些实施方案中约400-约2500MPa，和在一些实施方案中约600-约2000MPa）的纵向方向最大拉伸应力和约0.5-约50MPa（在一些实施方案中约1-约40MPa，在一些实施方案中约2-约20MPa）的横向方向最大拉伸应力。
在上面所述和图3-4中所示的实施方案中，可将长纤维在浸渍期间并入到挤出装置中，并因此变得与连续纤维混杂和通常分布遍及整个预浸料坯。然而应当认识到这样的构造不是必需的。在某些实施方案中，例如，可以将长纤维和连续纤维以它们形成单独的层的方式结合。在至少一部分长纤维延伸到连续纤维层的意义上讲，该层可以是“非离散的”。用于形成这样的非离散层状的预浸料坯的系统的一个实施方案可以包括另外的装置（例如挤出机），其用于将长纤维施加到用于浸渍连续纤维的模具的下游。以这种方式施加的长纤维仍无规地分布在预浸料坯中，但形成了单独的层。这更详细地示例于图6-7中。如所示，形成了含长纤维262的层260，并形成了含连续纤维272的层270。部分地由于其施加的方式，长纤维262的一部分230也可以延伸到连续纤维层270中。
当然，在基本上所有长纤维都包含在该层内的意义上讲，该层也可以是“离散的”。用于形成这样的离散层状预浸料坯的系统的一种实施方案示于图8中。在该特别的实施方案中，将预合并的连续纤维预浸料坯320从卷轴330上展开并在烘箱340(例如红外烘箱)内加热到热塑性基体的软化点或高于其软化点。然后，将软化的预浸料坯320供给到其中可以施加长纤维(未示出)的挤出装置350。然后可以将所得到的层状预浸料坯360供给到如上所述的两个合并辊筒290之间。再次，以这种方式施加的长纤维仍无规地分布在预浸料坯内，但形成了单独的“离散”层。这更详细地示例于图9-10中。如所示，形成了包含长纤维422的层420，形成了包含连续纤维424的层430。
V.由预浸料坯形成的制品
本发明的预浸料坯通常可以用于多种不同应用和部件中。例如，可以将预浸料坯制成型材、注模部件、压模部件等。“型材”是可具宽种类截面形状的中空或实体的拉挤部件，例如正方形、矩形、圆形、椭圆形、三角形、I形、C形、U形、J形、L形、槽型等。在中空型材中，该型材的至少一部分内部是空隙空间。该空隙空间可以任选地延伸该型材的整个长度。型材也可以是“线性的”达到沿型材的整个长度具有基本相同的截面形状的程度，或者它们可以具有变化的截面形状，例如弯曲、扭曲等。无论如何，这样的型材可以用作用于窗楣、装饰木板、栏杆、栏杆柱、屋顶瓦片、壁板(siding)、装饰板、管道、栅栏、立柱、灯柱、公路标志杆、路边标志杆等的结构部件。
由预浸料坯可以制备型材的方法可如本领域那些技术人员公知的变化。可以使用一个或多个预浸料坯层制备型材。参考图5，例如，显示了系统的一个特别实施方案，其中使用多个预浸料坯12制备型材。在该实施方案中，提供了在卷轴架20上的缠绕捆中的预浸料坯。卷轴架20可以是包括提供有各自支撑缠绕捆的水平旋转的纺轴22的框架的回卷卷轴架。也可以使用卷出卷轴架（pay-outcreel），特别是如果需要在纤维中引入扭曲的情况下。还应当认识到预浸料坯的形成也可以与型材的形成在线(in-line）形成。例如，在一个实施方案中，从图1中离开浸渍模具150的挤出物152可以直接供给用于形成型材的系统。
也可以使用拉伸调节装置40帮助控制拉伸程度。装置40可以包括位于与卷轴架20的旋转纺轴22平行的垂直平面上的入口板30。拉伸调节装置40可以包含以交错构造配置的圆柱形杆41，以使得预浸料坯12从这些杆的上下通过以限定波浪图案。可调节杆的高度以改变波浪图案的振幅并控制拉伸。
如果需要，可以将预浸料坯12在具有任意多种已知构造的烘箱45(例如红外烘箱、对流烘箱等)中加热。在加热期间，纤维单向取向以优化对热的暴露并在整个型材上维持均匀加热。条带12被加热的温度通常足够高以软化热塑性聚合物到条带能够结合在一起的程度。然而，温度没有如此高而导致破坏材料的整体性。例如温度可以为约100℃-约300℃，在一些实施方案中约110℃-约275℃，和在一些实施方案中约120℃-约250℃。在一个特别实施方案中，例如，使用丙烯腈-丁二烯-苯乙烯(ABS)作为聚合物，将条带加热到ABS的熔点(约为105℃)或熔点以上。在另一实施方案中，使用聚对苯二甲酸丁二醇酯(PBT)作为聚合物，将条带加热到PBT的熔点(约为224℃)或熔点以上。
一旦加热，可以将连续纤维条带12提供给合并模具以辅助将不同条带层结合在一起以及用于型材的最初形状的排列和形成。尽管本文涉及单个模具，但应当认识到合并模具50事实上可以由多个单独的模具（例如面板模具）形成。合并模具50可以接收预浸料坯12使其被引导沿着方向“A”通过模具50的通道（未示出）。该通道可以以多种取向和排列提供以产生所需的增强方案。在模具50内，预浸料坯通常保持在等于或高于条带中所用的热塑性基体的熔点的温度以确保充分的合并。
如果需要，也可以使用将预浸料坯压制成型材的最终形状的拉挤模具60。模具60的构造取决于所得到的型材所需的形状和性能。为了制备中空型材，拉挤模具典型地包含在其内部的心轴使得纤维材料在模具的内表面和心轴的外表面之间流动以形成所需的形状。此外，尽管本文涉及单个模具，但应当认识到拉挤模具60可以由多个单独的模具形成。
可以使用一个或多个层形成型材。在一个实施方案中，例如，使用在垂直方向上最初彼此间隔开的多个层。当它们通过合并模具50的各自通道时，该层的宽度任选地条带化，以有助于防止压力楔和保持连续纤维的排列和不扭曲。尽管未具体显示，也可以在合并模具50的内部提供心轴以帮助引导该层在型材的至少一个侧面上彼此接触。例如，预浸料坯层的一个侧面和另一预浸料坯层的侧面可以成一定角度使得它们彼此接触并形成中空型材的侧面。然而，型材的另一侧面典型地在合并模具50内保持敞开以使得随后可将长纤维材料施加到拉挤模具内型材的内部。当在所需位置时，如上所述将预浸料坯层牵引出拉挤模具60。
如果需要，可以用覆盖层施加在所得到的型材上以增强型材的审美外观和/或保护其不受环境条件的影响。参考图5，例如，可以通过以任意所需角度取向的挤出机施加这样的覆盖层以将热塑性树脂引入到在覆盖模具72中。该树脂可以包含本领域中已知的且通常与用于形成型材的热塑性聚合物相容的任意适合的热塑性聚合物。适合的覆盖聚合物可以包括例如：丙烯酸类聚合物、聚氯乙烯（PVC）、聚对苯二甲酸丁二醇酯（PBT）、ABS、聚烯烃、聚酯、聚缩醛、聚酰胺、聚氨酯等。尽管覆盖树脂通常不含纤维，然而其可以包含其它添加剂用以提高型材的最终性能。在该阶段使用的添加剂材料可以包括不适合于并入连续纤维层或长纤维层中的那些。例如在复合材料结构中添加颜料以降低成型制品的完成劳动力可能是所需的，或者在复合材料结构中添加阻燃剂以提高成型制品的阻燃特征可能是所需的。因为很多添加剂材料是热敏性的，因此过多的热量可能引起它们分解而产生挥发性气体。因此，如果在高热条件下将热敏性添加剂材料与浸渍树脂挤出，结果可能是添加剂材料的完全降解。添加剂材料例如可以包括：矿物增强剂、润滑剂、阻燃剂、发泡剂、起泡剂、抗紫外光剂、热稳定剂、颜料及其组合。适合的矿物增强剂可以包括例如：碳酸钙、二氧化硅、云母、粘土、滑石、硅酸钙、石墨、硅酸钙、三水合氧化铝、铁酸钡及其组合。
尽管本文未详细示出，覆盖模具72可以包含现有技术中已知的各种特征以帮助实现覆盖层的所需应用。例如，覆盖模具72可以具有使进入的型材排列的入口导向装置。覆盖模具也可以包含加热机构（例如加热板），其在施加覆盖层之前对型材进行预加热以帮助确保充分结合。
在任选的覆盖之后，如本领域中已知可以将成型部件15供给到冷却系统80。冷却系统80例如可以是真空定型机(sizer)，其包含在随其冷却时当真空对着其壁将热成型件牵引出时完全将型材封装的一个或多个模块（例如铝模块）。可以在定型机上施加冷却介质，例如空气或水，以将型材固化成适当的形状。
在任选的覆盖之后，然后如本领域已知最后使用冷却系统80冷却成型部件。冷却系统80例如可以是真空定型机，其包含在随其冷却时当真空对着其壁将热成型件牵引出时完全将型材封装的一个或多个模块（例如铝模块）。可以在定型机上施加冷却介质，例如空气或水，以将型材固化成适当的形状。
在形成型材时典型地使用真空定型机。然而，即使没有使用真空定型机，在其离开覆盖模具（或者如果在没有施加覆盖时离开合并或定标模具）之后冷却型材通常是所需的。可以使用本领域已知的任意技术（例如真空水槽、冷却空气流或空气喷射、冷却夹套、内部冷却通道、冷却流体循环通道等）进行冷却。无论如何，通常控制材料的冷却温度以实现最佳的机械性能、部件尺寸公差、良好加工和审美合意的复合材料。例如，如果冷却位置的温度过高，材料可能在工具中膨胀并干扰工艺。对于半结晶材料，过低的温度同样地可造成材料过快地冷却下降且不允许完全结晶，由此对复合材料的机械和耐化学性造成危害。可使用具有独立温度控制的多个冷却模具段以提供加工和性能特征之间的最佳平衡。在一个特别的实施方案中，例如，使用温度保持在约10℃-约50℃和在一些实施方案中约15℃-约35℃的真空水槽。
如所认识到的，当型材向前通过本发明的系统的任意段时可控制其温度以实现最佳的制造和所需的最终的复合材料性能。使用筒形电加热器、循环流体冷却等或对本领域那些技术人员已知的任何其它温度可控制装置控制任意或所有组件部分的温度。
再次参考图5，牵引装置82位于冷却系统80的下游，其将成品型材16牵引通过系统用于复合材料的最终定型。牵引装置82可以是能够将型材以所需速率牵引通过加工系统的任何装置。典型的牵引装置包括例如：履带式牵引器和往复式牵引器。如果所需，也可以使用一个或多个定标模具(未示出)。这样的模具包含切割到精确的型材形状的开口，从最初过大的尺寸逐渐变为最终型材形状。当型材通过其中时，抵消了其移动或松垂的任何趋势，并将其推回(重复地)到其正确的形状。一旦定型，可以将型材在切割位置（未示出）切割成所需的尺寸，例如用能够进行截面切割的截断锯。
图11中更详细地显示了由上述方法制成的作为元件516的型材的一个实施方案。如所示，型材516具有通常为矩形的形状且由其中分布了多个长纤维518的条带514制成。条带514可以由本发明的一个或多个预浸料坯制成。覆盖层519也围着条带514的周围延伸且限定了型材516的外表面。条带的厚度可合理地选择以帮助实现型材的特定的拉伸强度和横向强度(例如弯曲模量)。例如，条带可以具有约1.0-约4.0毫米和在一些实施方案中约2.0-约3.0毫米的厚度。覆盖层519的厚度取决于所需的部件功能，但典型地为约0.1-约5毫米和在一些实施方案中约0.2-约3毫米。
如所认识到的，上述具体的型材实施方案仅是由本发明可做出的多种设计的示例。在多种可能的型材设计中，应当认识到除了上述的那些还可以使用另外的连续纤维和/或长纤维材料层。
除了拉挤之外，也可以使用其它系统将预浸料坯加工成所需的制品。例如，可以使用注模系统，其包含其中可以设置一个或多个预浸料坯的模具。可以控制并优化注射器内的时间使得热塑性树脂不会预固化。当达到循环时间且桶充满用于排出时，可以使用活塞将材料注入模具空腔。在本发明中也可使用压模系统。如同注模一样，将预浸料坯成型为所需的制品也发生在模具内。可以使用任何已知的技术(例如通过用自动机器人手臂拾取)将预浸料坯置于压缩模具内。模具的温度可以维持在等于或高于热塑性树脂的固化温度的温度并持续允许固化的所需时间段。然后可以通过将其调到熔融温度以下的温度将模制产品固化。可以将得到的产品脱模。可以调节各模制工艺的循环时间以适合使用的树脂，从而实现充分的结合并提高总工艺生产率。
上述系统中所用的模具可以是单空腔或多空腔的模具。空腔的数量可以由使用的树脂、循环时间和所需的输出速率决定。可以选择模具的形状以制备用于具体应用的产品，例如侧板(sidingpanels)、栅栏桩部件、端盖、接头、合叶、用于内部和外部装饰的装饰板、合成屋顶板、石板、盖板(shakes)或面板等。
在不偏离本发明的精神和范围的情况下，本领域的普通技术人员可以实施本发明的这些和其它修改和变化。此外，应当认识到多种实施方案的各方面可以全部地或部分地互换。此外，本领域的那些普通技术人员将认识到之前的描述仅是示例的方式，并不意于限制在这样的所附权利要求书中如此进一步描述的本发明。

Claims (25)

1.一种热塑性预浸料坯，所述热塑性预浸料坯包含：
基本上取向在纵向方向上的多个连续纤维，所述连续纤维构成所述预浸料坯的10wt％-80wt％；
多个无规分布的长纤维，至少一部分以相对于纵向方向成一定角度取向，所述长纤维构成所述预浸料坯的2wt％-35wt％；和
树脂基体，包含一种或多种热塑性聚合物且所述连续纤维和所述长纤维嵌入其中，其中所述热塑性聚合物构成所述预浸料坯的10wt％-80wt％；
其中所述预浸料坯的纵向方向上最大拉伸应力与所述预浸料坯的横向方向上最大拉伸应力之比为1-40；和
其中所述长纤维与所述连续纤维混杂；或其中所述长纤维存在于所述预浸料坯的第一层内，所述连续纤维存在于所述预浸料坯的第二层内；和至少一部分所述长纤维延伸到所述第二层中。
2.权利要求1的热塑性预浸料坯，其中所述预浸料坯的纵向方向上最大拉伸应力与所述预浸料坯的横向方向上最大拉伸应力之比为2-30。
3.权利要求1的热塑性预浸料坯，其中所述预浸料坯呈现出250-3000兆帕的纵向方向上最大拉伸应力。
4.权利要求1的热塑性预浸料坯，其中所述预浸料坯呈现出0.5-50兆帕的横向方向上最大拉伸应力。
5.权利要求1的热塑性预浸料坯，其中所述连续纤维构成预浸料坯的20wt％-70wt％。
6.权利要求1的热塑性预浸料坯，其中所述长纤维构成预浸料坯的5wt％-30wt％。
7.权利要求1的热塑性预浸料坯，其中所述连续纤维、长纤维或两者包括玻璃纤维、碳纤维或玻璃纤维和碳纤维的组合。
8.权利要求1的热塑性预浸料坯，其中所述热塑性聚合物包括聚烯烃、聚醚酮、聚醚酰亚胺、聚亚芳基酮、液晶聚合物、聚芳硫醚、含氟聚合物、聚缩醛、聚氨酯、聚碳酸酯、苯乙烯类聚合物、聚酯、聚酰胺或其组合。
9.权利要求1的热塑性预浸料坯，其中所述预浸料坯具有2％或更小的空隙率。
10.包含权利要求1的预浸料坯的线状型材。
11.权利要求10的线状型材，其中所述型材进一步包含限定所述型材表面的覆盖层。
12.包含权利要求1的预浸料坯的模制品。
13.热塑性预浸料坯的制备方法，所述方法包括：
将连续纤维和长纤维供给到挤出装置；
将热塑性进料供给到挤出装置，其中所述进料包含至少一种热塑性聚合物；和
将所述连续纤维、长纤维和热塑性聚合物在浸渍模具内挤出以形成其中所述连续纤维与所述长纤维混杂并用热塑性聚合物基体嵌入的挤出物。
14.权利要求13的方法，其中所述进料包含所述长纤维。
15.权利要求13的方法，还包括将挤出物牵引通过限定在辊筒之间的辊隙以将挤出物合并成薄片状。
16.权利要求13的方法，其中所述连续纤维构成所述预浸料坯的10wt％-80wt％，和所述长纤维构成所述预浸料坯的2wt％-35wt％。
17.权利要求13的方法，其中所述连续纤维、长纤维或两者包括玻璃纤维、碳纤维或玻璃纤维和碳纤维的组合。
18.权利要求13的方法，其中所述热塑性聚合物包括聚烯烃、聚醚酮、聚醚酰亚胺、聚亚芳基酮、液晶聚合物、聚芳硫醚、含氟聚合物、聚缩醛、聚氨酯、聚碳酸酯、苯乙烯类聚合物、聚酯、聚酰胺或其组合。
19.权利要求13的方法，其中歧管组件将所述热塑性进料供给到挤出装置，所述歧管组件包括热塑性进料流动通过其的分岔浇口。
20.热塑性预浸料坯的制备方法，所述方法包括：
将连续纤维供给到挤出装置；
将热塑性进料供给到挤出装置，其中所述进料包含至少一种热塑性聚合物；和
将所述连续纤维和所述进料在浸渍模具中挤出以形成其中用热塑性聚合物的基体嵌入连续纤维的挤出物；
然后将长纤维施加到所述挤出物以形成复合材料
其中所述长纤维存在于所述预浸料坯的第一层内，所述连续纤维存在于所述预浸料坯的第二层内；和至少一部分所述长纤维延伸到所述第二层中。
21.权利要求20的方法，还包括将所述复合材料牵引通过限定在辊筒之间的辊隙以将复合材料合并成薄片状。
22.权利要求20的方法，其中所述连续纤维构成构成所述预浸料坯的10wt％-80wt％，和所述长纤维构成所述预浸料坯的2wt％-35wt％。
23.权利要求20的方法，其中所述连续纤维、长纤维或两者包括玻璃纤维、碳纤维或玻璃纤维和碳纤维的组合。
24.权利要求20的方法，其中所述热塑性聚合物包括聚烯烃、聚醚酮、聚醚酰亚胺、聚亚芳基酮、液晶聚合物、聚芳硫醚、含氟聚合物、聚缩醛、聚氨酯、聚碳酸酯、苯乙烯类聚合物、聚酯、聚酰胺或其组合。
25.权利要求20的方法，其中歧管组件将热塑性进料供给挤出装置，歧管组件包括热塑性进料流动通过其的分岔浇口。
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