CN100488769C - 无机片材层合材料 - Google Patents

无机片材层合材料 Download PDF

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Publication number
CN100488769C
CN100488769C CNB2004800067769A CN200480006776A CN100488769C CN 100488769 C CN100488769 C CN 100488769C CN B2004800067769 A CNB2004800067769 A CN B2004800067769A CN 200480006776 A CN200480006776 A CN 200480006776A CN 100488769 C CN100488769 C CN 100488769C
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China
Prior art keywords
laminate
inorganic
sheet
paper
inorganic sheet
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Expired - Lifetime
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CNB2004800067769A
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CN1759011A (zh
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D·W·安德森
D·W·考卡
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DuPont Safety and Construction Inc
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EI Du Pont de Nemours and Co
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    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B27/00—Layered products comprising a layer of synthetic resin
    • B32B27/06—Layered products comprising a layer of synthetic resin as the main or only constituent of a layer, which is next to another layer of the same or of a different material
    • B32B27/10—Layered products comprising a layer of synthetic resin as the main or only constituent of a layer, which is next to another layer of the same or of a different material of paper or cardboard
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B27/00—Layered products comprising a layer of synthetic resin
    • B32B27/36—Layered products comprising a layer of synthetic resin comprising polyesters
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B25—HAND TOOLS; PORTABLE POWER-DRIVEN TOOLS; MANIPULATORS
    • B25B—TOOLS OR BENCH DEVICES NOT OTHERWISE PROVIDED FOR, FOR FASTENING, CONNECTING, DISENGAGING OR HOLDING
    • B25B13/00—Spanners; Wrenches
    • B25B13/48—Spanners; Wrenches for special purposes
    • B25B13/50—Spanners; Wrenches for special purposes for operating on work of special profile, e.g. pipes
    • B25B13/5008—Spanners; Wrenches for special purposes for operating on work of special profile, e.g. pipes for operating on pipes or cylindrical objects
    • B25B13/5083—Spanners; Wrenches for special purposes for operating on work of special profile, e.g. pipes for operating on pipes or cylindrical objects by internally gripping the pipe
    • B—PERFORMING OPERATIONS; TRANSPORTING
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    • B32B27/00—Layered products comprising a layer of synthetic resin
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    • B32B37/14—Methods or apparatus for laminating, e.g. by curing or by ultrasonic bonding characterised by the properties of the layers
    • B32B37/15—Methods or apparatus for laminating, e.g. by curing or by ultrasonic bonding characterised by the properties of the layers with at least one layer being manufactured and immediately laminated before reaching its stable state, e.g. in which a layer is extruded and laminated while in semi-molten state
    • B32B37/153—Methods or apparatus for laminating, e.g. by curing or by ultrasonic bonding characterised by the properties of the layers with at least one layer being manufactured and immediately laminated before reaching its stable state, e.g. in which a layer is extruded and laminated while in semi-molten state at least one layer is extruded and immediately laminated while in semi-molten state
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    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01B—CABLES; CONDUCTORS; INSULATORS; SELECTION OF MATERIALS FOR THEIR CONDUCTIVE, INSULATING OR DIELECTRIC PROPERTIES
    • H01B3/00—Insulators or insulating bodies characterised by the insulating materials; Selection of materials for their insulating or dielectric properties
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  • Physics & Mathematics (AREA)
  • Spectroscopy & Molecular Physics (AREA)
  • Engineering & Computer Science (AREA)
  • Mechanical Engineering (AREA)
  • Laminated Bodies (AREA)
  • Insulating Bodies (AREA)
  • Extrusion Moulding Of Plastics Or The Like (AREA)

Abstract

一种由无机片材和聚酯树脂的层合材料，其总厚度为5～25密耳，其横向和纵向两者的断裂伸长为至少25%。

Description

无机片材层合材料
技术领域
本发明涉及一种包含无机片材和聚酯聚合物的改性层合材料，优选通过聚酯聚合物层分隔开的两层无机片材的层合材料.
背景技术
这种无机片材层合材料用于变压器和其它电气设备，在其中层合材料用作介电绝缘材料。这类层合材料需要具有折叠耐久性和韧性。需要进行层合材料内粘附或这类层合材料的撕裂性能或断裂伸长性能方面的任何改性。
发明概述
本发明涉及一种由无机片材和聚酯树脂的层合材料，其总厚度为5～25密耳，在横向和纵向两者的断裂伸长为至少25％.优选，横向断裂伸长为至少30％.在本发明的一个实施方案中，在层合材料中的树脂层厚度能够大于在层合材料中的任何单个非织造片材的厚度.优选，非织造无机片材是纸，所述纸包括无机矿物质如硅酸铝，无机增强材料如玻璃纤维，和粘合剂如丙烯腈胶乳.优选用于层合材料的聚酯树脂是聚对苯二甲酸乙二酯和聚萘二甲酸乙二酯.
附图说明
图1是用于制造本发明层合材料的挤出层合工艺的简要图示.
图2是，与现有技术粘合层合材料相比较，本发明挤出层合材料的初始抗撕裂性的改进.
具体实施方式
由无机片材或纸和聚酯树脂薄膜制造的层合材料已经用于变压器和其它电气设备，在其中层合材料用作介电绝缘材料.要求这类绝缘层合材料具有特别适于变压器制造商要求的物理性能的组合。这些性能包括：除了绝缘性能之外，还有其它机械性能，后者包括初始抗撕裂性(如通过断裂伸长所测定的)和高抗撕裂蔓延性(如通过平均撕裂负荷所测定的).这些性能在评价绝缘层合材料中是特别有用的，原因在于：在制造变压器中，可能发生在组装期间会损坏绝缘层合材料的问题.
现已发现，无机绝缘层合材料的伸长和撕裂性能能够通过更换用于层合材料的聚酯的类型进行改善.尤其是，现已发现，用熔融聚酯树脂制造的层合材料与用薄膜制造的层合材料相比，具有改善的伸长和撕裂性能.
典型地，现有技术用于电气绝缘的层合材料具有已应用的聚酯薄膜.因为聚酯薄膜自身没有对无机片材的良好粘附性，已经应用粘合剂将薄膜固定到无机片材上。将薄膜固定到无机片材的方法包括：首先将粘合剂涂布到薄膜上，然后在高温下层合已涂布的薄膜于无机片材上.相信，在层合材料中以薄膜形式应用聚酯限制了最终层合材料的伸长和撕裂性能，因为形成固体薄膜的典型工艺赋予聚酯层以结晶度和取向.认为这样会降低最终层合材料的挠曲性、韧性和抗撕裂性.
本发明的层合材料使用无机片材或纸，这些术语被意欲在本发明中可互换使用.在本发明使用的片材或纸能够采用传统造纸工艺、设备和方法来制造.术语“横向”和“纵向”在本领域中众所周知，指的是在测量物理性能的片材中的正交方向；纵向与纸机卷绕方向平行，而横向则横切纸机.本发明无机纸能够含有矿物组分、无机增强组分和粘合剂。这些组分在水悬浮液中混合，浇注在筛网上，在其上使它们脱水、任选受压和干燥。这些片材的层能够组合成某种厚度的纸，这些纸能够经压光或其它致密工艺压实.用于制造用于本发明的无机纸和片材的矿物和/或无机材料包括但不限于玻璃、硅酸铝和/或这些与其它无机填料的混合物；这些无机材料可以以纤维形式存在.有用的粘合剂包括但不限于丙烯腈胶乳.本发明的优选层合材料制造自市购自Quin-T公司(Tilton，NH)的
Figure C200480006776D0004101207QIETU
和无机片材.
对于无机片材的厚度没有严格要求，其依赖于层合材料的最终应用以及最终层合材料中所使用的无机层的层数.虽然本发明可以使用两层，即，一个无机层和一个聚合物层，和优选使用三层，即，两个无机片材层和一个聚合物层，但是总会理解，对最终制品中能够存在的其它材料或层数没有高限.
本文使用的术语无机意指，主要成分是不含烃的粘土、纤维、片状粉末、粒状或其它结构，特别是天然矿物如硅酸铝，和加工的无机材料如玻璃纤维.
在本发明中施加到无机片材的优选聚合物是聚对苯二甲酸乙二酯(PET)和聚萘二甲酸乙二酯(PEN)。这些聚合物可以包括种种共聚单体，包括二甘醇、环己烷二甲醇、聚乙二醇、戊二酸、壬二酸、癸二酸和间苯二甲酸等.除了这些共聚单体之外，可以使用支化剂如1，3，5-苯三酸、均苯四酸、三羟甲基丙烷和三羟甲基乙烷以及季戊四醇.PET可以通过已知聚合工艺从或者对苯二甲酸或其低级烷基酯(如对苯二甲酸二甲酯)和乙二醇或这些的共混物或混合物制得.PEN可以通过已知聚合工艺从2，6-萘二羧酸和乙二醇制得.
制造本发明层合材料的一种方法包括：挤出熔融聚合物于两层无机片材之间，随后施压和骤冷形成层合材料.能够以任何方式将熔融树脂挤出到无机片材上.例如，可先将树脂挤出到一个无机片材上，然后采用第二无机片材覆盖上，再使用施压辊或层合辊层合.参见图1，在一种优选方法中，将熔融树脂从挤出机施加到缝口模头1中.将缝口模头定向，使熔融树脂片材以向下方式挤出到一组水平层合辊2上.无机片材3的两个供料辊提供两个单独的无机片材料片4到层合辊，两个料片和熔融树脂片材全部在层合辊辊隙相遇，树脂在两个料片之间定位.层合辊将料片和树脂压固在一起；然后采用一组冷却辊5使压固的层合材料骤冷.然后可以切割层合材料为应用所需要的适宜尺寸.
在本发明的另一个实施方案中，熔融聚合物组合可以以使不同聚合物在两个无机片材之间成层的方式挤出.例如，聚合物层能由三层组成，例如，依次，一层为具有第一特性粘度的PET聚合物，一层为具有第二特性粘度的PET聚合物，和第三层为具有与第一层相同的特性粘度的PET聚合物。以这样一种方式，能够使用对无机片材具有较大亲合力的PET聚合物，将对无机片材具有较小亲合力的PET聚合物并合入层合材料.
本发明的层合材料厚度为5～25密耳，横向和纵向断裂伸长为至少25％.本发明的优选层合材料横向断裂伸长为至少30％，纵向断裂伸长为至少25％.一般说，这类层合材料的树脂厚度大于层合材料中的任何一个无机片材的厚度.
在下述实施例中，所有份数和百分数均按重量计，除非另外指出.初始抗撕裂性按照ASTM D1004借助断裂伸长测定.抗撕裂蔓延性按照ASTM D1938借助平均撕裂负荷测定。
实施例1
该实施例说明在没有粘合剂的条件下将无机纸层合到聚酯聚合物上所遇到的问题和通过本发明获得的粘附.在该实施例中使用两类片材：市购无机纸(具体地说，Quin-T公司制造的
Figure C200480006776D00061
)和高压光间位芳族聚酰胺纸载体片材，结果熔融聚酯聚合物总不能粘附于其上.
按照如下所述采用热压机将具有0.60 d1/g特性粘度的聚对苯二甲酸乙二酯聚酯层合在两个纸片材组合之间.为了将聚酯聚合物粘附到无机纸上，不需要对纸表面施加粘合剂、化学、火焰、热或电晕处理或者类似的活化.热压机条件示于表1中.
试验A：将聚酯聚合物小粒料置于两个无机片材之间并将所述组合置于热压机.使聚酯粒料熔融并在片材之间流动.在无机片材中所用的粘合剂也熔融并流动，使片材和聚合物的组合溶解到不合用的层合材料中.
试验B：将聚酯聚合物小粒料置于两个无机片材之间并将所述组合置于热压机，但比试验A的时间短.使聚酯粒料熔融并在片材之间流动。在无机片材中所用的粘合剂也熔融并流动但片材和聚合物的组合保持其完整性.然而，所得层合材料是脆的并且实际上是不可利用的。
试验C：将聚酯聚合物小粒料置于未闭合热压机中一个间位芳族聚酰胺片材上.在未闭合热压机中5min之后，聚合物粒料熔融并在芳族聚酰胺片材表面上流动.在将芳族聚酰胺片材和熔融聚酯聚合物从压机中取出之后，和在聚合物仍然熔融的同时，将一个无机纸片材手工压到熔融聚酯聚合物表面上.立即将所得层合材料骤冷，防止在无机片材中应用的粘合剂熔融.注意到在无机片材和聚酯聚合物之间粘附优良，无机片材没有脆化。
表1
Figure C200480006776D00071
实施例2
该实施例说明通过挤出层合制造的本发明层合材料的性能，并与粘合层合制造的层合材料进行比较.挤出层合材料按下述制造.无机纸(具体地说，Quin-T公司制造的
Figure C200480006776D00072
)以市购形式应用.将熔融聚对苯二甲酸乙二酯(PET)聚合物，以三层组合的形式或者以共挤出PET聚合物形式，分别通过将聚酯聚合物挤出层合到两层纸之间施加到纸表面上，所用PET聚合物分别特性粘度为0.65/0.85/0.65d1/g.为了将聚酯聚合物粘附到无机纸上，不需要对纸表面进行粘合剂、化学、火焰、热或电晕处理或者相似的活化.将这些挤出层合材料与用于电气绝缘的市购粘合剂层合材料进行比较，后者含有粘合层合在两层无机纸之间的聚酯薄膜(制造自和市购自Quin-T公司的
Figure C200480006776D00073
层合材料).
按照ASTM D1004(塑料薄膜和片材的初始抗撕裂性的测试方法)和ASTM D1938(通过单一撕裂方法进行的关于塑料薄膜和片材的抗撕裂蔓延性的测试方法)检测以此方式生产的层合材料样品，评价所得撕裂性能.
在所有试验中，聚酯聚合物和无机纸之间的粘合剂粘合高于纸的内在强度.表2中所示的数据说明：本发明的通过挤出层合制造的层合材料具有改进的初始抗撕裂性和改进的抗撕裂蔓延性，初始抗撕裂性如所测定的，具有30％以上横向断裂伸长，而纵向为25％以上。在下文所使用的，EL代表挤出层合，AL代表粘合剂层合，MD代表纵向，XD代表横向.图2说明这些层合材料断裂伸长的改进，线10和15表示挤出层合材料的MD和XD值，线20和25表示粘合剂层合材料的MD和XD值.
表2
Figure C200480006776D00081

Claims (3)

1.一种制造用于电气绝缘的层合材料的方法，包括：
a)将两层无机片材提供到在一对辊之间的辊隙中，
b)将熔融聚酯聚合物挤出在这对辊之间的辊隙前或辊隙中的无机片之间或之上，
c)将无机片材和熔融聚合物压固在所述辊之间，形成未骤冷的层合材料，和
d)冷却未骤冷的层合材料以形成骤冷的层合材料，从而得到一种层合片材，其总厚度为5～25密耳，在横向和纵向两者的断裂伸长为至少25％。
2.权利要求1的方法，其中该熔融聚酯聚合物经缝口模头挤出。
3.权利要求1的方法，其中熔融聚酯聚合物包括成层的聚酯聚合物组合。
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