CN101056758A - 覆金属箔层叠体及其制造方法 - Google Patents

覆金属箔层叠体及其制造方法 Download PDF

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Publication number
CN101056758A
CN101056758A CNA2005800383953A CN200580038395A CN101056758A CN 101056758 A CN101056758 A CN 101056758A CN A2005800383953 A CNA2005800383953 A CN A2005800383953A CN 200580038395 A CN200580038395 A CN 200580038395A CN 101056758 A CN101056758 A CN 101056758A
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Prior art keywords
liquid crystal
crystal polymer
metal
film
thermoplastic liquid
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CN101056758B (zh
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小野寺稔
吉川淳夫
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Kuraray Co Ltd
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Kuraray Co Ltd
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    • 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
    • B32B37/00—Methods or apparatus for laminating, e.g. by curing or by ultrasonic bonding
    • B32B37/14—Methods or apparatus for laminating, e.g. by curing or by ultrasonic bonding characterised by the properties of the layers
    • B32B37/16—Methods or apparatus for laminating, e.g. by curing or by ultrasonic bonding characterised by the properties of the layers with all layers existing as coherent layers before laminating
    • B32B37/20—Methods or apparatus for laminating, e.g. by curing or by ultrasonic bonding characterised by the properties of the layers with all layers existing as coherent layers before laminating involving the assembly of continuous webs only
    • 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
    • B32B15/00—Layered products comprising a layer of metal
    • B32B15/04—Layered products comprising a layer of metal comprising metal as the main or only constituent of a layer, which is next to another layer of the same or of a different material
    • B32B15/08—Layered products comprising a layer of metal comprising metal as the main or only constituent of a layer, which is next to another layer of the same or of a different material of synthetic resin
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
    • B29C—SHAPING OR JOINING OF PLASTICS; SHAPING OF MATERIAL IN A PLASTIC STATE, NOT OTHERWISE PROVIDED FOR; AFTER-TREATMENT OF THE SHAPED PRODUCTS, e.g. REPAIRING
    • B29C65/00—Joining or sealing of preformed parts, e.g. welding of plastics materials; Apparatus therefor
    • B29C65/02—Joining or sealing of preformed parts, e.g. welding of plastics materials; Apparatus therefor by heating, with or without pressure
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
    • B29C—SHAPING OR JOINING OF PLASTICS; SHAPING OF MATERIAL IN A PLASTIC STATE, NOT OTHERWISE PROVIDED FOR; AFTER-TREATMENT OF THE SHAPED PRODUCTS, e.g. REPAIRING
    • B29C65/00—Joining or sealing of preformed parts, e.g. welding of plastics materials; Apparatus therefor
    • B29C65/02—Joining or sealing of preformed parts, e.g. welding of plastics materials; Apparatus therefor by heating, with or without pressure
    • B29C65/44—Joining a heated non plastics element to a plastics element
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
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    • B29C66/00—General aspects of processes or apparatus for joining preformed parts
    • B29C66/01—General aspects dealing with the joint area or with the area to be joined
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    • B29C66/10—Particular design of joint configurations particular design of the joint cross-sections
    • B29C66/11—Joint cross-sections comprising a single joint-segment, i.e. one of the parts to be joined comprising a single joint-segment in the joint cross-section
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    • B29C66/9141—Measuring or controlling the joining process by measuring or controlling the temperature, the heat or the thermal flux by controlling or regulating the temperature, the heat or the thermal flux by controlling or regulating the temperature
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    • B29C66/9141—Measuring or controlling the joining process by measuring or controlling the temperature, the heat or the thermal flux by controlling or regulating the temperature, the heat or the thermal flux by controlling or regulating the temperature
    • B29C66/91421—Measuring or controlling the joining process by measuring or controlling the temperature, the heat or the thermal flux by controlling or regulating the temperature, the heat or the thermal flux by controlling or regulating the temperature of the joining tools
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
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    • B29C66/90—Measuring or controlling the joining process
    • B29C66/91—Measuring or controlling the joining process by measuring or controlling the temperature, the heat or the thermal flux
    • B29C66/914—Measuring or controlling the joining process by measuring or controlling the temperature, the heat or the thermal flux by controlling or regulating the temperature, the heat or the thermal flux
    • B29C66/9161—Measuring or controlling the joining process by measuring or controlling the temperature, the heat or the thermal flux by controlling or regulating the temperature, the heat or the thermal flux by controlling or regulating the heat or the thermal flux, i.e. the heat flux
    • B29C66/91641—Measuring or controlling the joining process by measuring or controlling the temperature, the heat or the thermal flux by controlling or regulating the temperature, the heat or the thermal flux by controlling or regulating the heat or the thermal flux, i.e. the heat flux the heat or the thermal flux being non-constant over time
    • B29C66/91643—Measuring or controlling the joining process by measuring or controlling the temperature, the heat or the thermal flux by controlling or regulating the temperature, the heat or the thermal flux by controlling or regulating the heat or the thermal flux, i.e. the heat flux the heat or the thermal flux being non-constant over time following a heat-time profile
    • B29C66/91645—Measuring or controlling the joining process by measuring or controlling the temperature, the heat or the thermal flux by controlling or regulating the temperature, the heat or the thermal flux by controlling or regulating the heat or the thermal flux, i.e. the heat flux the heat or the thermal flux being non-constant over time following a heat-time profile by steps
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
    • B29C—SHAPING OR JOINING OF PLASTICS; SHAPING OF MATERIAL IN A PLASTIC STATE, NOT OTHERWISE PROVIDED FOR; AFTER-TREATMENT OF THE SHAPED PRODUCTS, e.g. REPAIRING
    • B29C66/00—General aspects of processes or apparatus for joining preformed parts
    • B29C66/90—Measuring or controlling the joining process
    • B29C66/91—Measuring or controlling the joining process by measuring or controlling the temperature, the heat or the thermal flux
    • B29C66/919—Measuring or controlling the joining process by measuring or controlling the temperature, the heat or the thermal flux characterised by specific temperature, heat or thermal flux values or ranges
    • B29C66/9192—Measuring or controlling the joining process by measuring or controlling the temperature, the heat or the thermal flux characterised by specific temperature, heat or thermal flux values or ranges in explicit relation to another variable, e.g. temperature diagrams
    • B29C66/91921—Measuring or controlling the joining process by measuring or controlling the temperature, the heat or the thermal flux characterised by specific temperature, heat or thermal flux values or ranges in explicit relation to another variable, e.g. temperature diagrams in explicit relation to another temperature, e.g. to the softening temperature or softening point, to the thermal degradation temperature or to the ambient temperature
    • B29C66/91931—Measuring or controlling the joining process by measuring or controlling the temperature, the heat or the thermal flux characterised by specific temperature, heat or thermal flux values or ranges in explicit relation to another variable, e.g. temperature diagrams in explicit relation to another temperature, e.g. to the softening temperature or softening point, to the thermal degradation temperature or to the ambient temperature in explicit relation to the fusion temperature or melting point of the material of one of the parts to be joined
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
    • B29C—SHAPING OR JOINING OF PLASTICS; SHAPING OF MATERIAL IN A PLASTIC STATE, NOT OTHERWISE PROVIDED FOR; AFTER-TREATMENT OF THE SHAPED PRODUCTS, e.g. REPAIRING
    • B29C66/00—General aspects of processes or apparatus for joining preformed parts
    • B29C66/90—Measuring or controlling the joining process
    • B29C66/91—Measuring or controlling the joining process by measuring or controlling the temperature, the heat or the thermal flux
    • B29C66/919—Measuring or controlling the joining process by measuring or controlling the temperature, the heat or the thermal flux characterised by specific temperature, heat or thermal flux values or ranges
    • B29C66/9192—Measuring or controlling the joining process by measuring or controlling the temperature, the heat or the thermal flux characterised by specific temperature, heat or thermal flux values or ranges in explicit relation to another variable, e.g. temperature diagrams
    • B29C66/91921—Measuring or controlling the joining process by measuring or controlling the temperature, the heat or the thermal flux characterised by specific temperature, heat or thermal flux values or ranges in explicit relation to another variable, e.g. temperature diagrams in explicit relation to another temperature, e.g. to the softening temperature or softening point, to the thermal degradation temperature or to the ambient temperature
    • B29C66/91931—Measuring or controlling the joining process by measuring or controlling the temperature, the heat or the thermal flux characterised by specific temperature, heat or thermal flux values or ranges in explicit relation to another variable, e.g. temperature diagrams in explicit relation to another temperature, e.g. to the softening temperature or softening point, to the thermal degradation temperature or to the ambient temperature in explicit relation to the fusion temperature or melting point of the material of one of the parts to be joined
    • B29C66/91933—Measuring or controlling the joining process by measuring or controlling the temperature, the heat or the thermal flux characterised by specific temperature, heat or thermal flux values or ranges in explicit relation to another variable, e.g. temperature diagrams in explicit relation to another temperature, e.g. to the softening temperature or softening point, to the thermal degradation temperature or to the ambient temperature in explicit relation to the fusion temperature or melting point of the material of one of the parts to be joined higher than said fusion temperature
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
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    • B29C66/90—Measuring or controlling the joining process
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    • B29C66/91931—Measuring or controlling the joining process by measuring or controlling the temperature, the heat or the thermal flux characterised by specific temperature, heat or thermal flux values or ranges in explicit relation to another variable, e.g. temperature diagrams in explicit relation to another temperature, e.g. to the softening temperature or softening point, to the thermal degradation temperature or to the ambient temperature in explicit relation to the fusion temperature or melting point of the material of one of the parts to be joined
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    • H—ELECTRICITY
    • H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
    • H05K—PRINTED CIRCUITS; CASINGS OR CONSTRUCTIONAL DETAILS OF ELECTRIC APPARATUS; MANUFACTURE OF ASSEMBLAGES OF ELECTRICAL COMPONENTS
    • H05K1/00—Printed circuits
    • H05K1/02—Details
    • H05K1/03—Use of materials for the substrate
    • H05K1/0313—Organic insulating material
    • H—ELECTRICITY
    • H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
    • H05K—PRINTED CIRCUITS; CASINGS OR CONSTRUCTIONAL DETAILS OF ELECTRIC APPARATUS; MANUFACTURE OF ASSEMBLAGES OF ELECTRICAL COMPONENTS
    • H05K3/00—Apparatus or processes for manufacturing printed circuits
    • H—ELECTRICITY
    • H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
    • H05K—PRINTED CIRCUITS; CASINGS OR CONSTRUCTIONAL DETAILS OF ELECTRIC APPARATUS; MANUFACTURE OF ASSEMBLAGES OF ELECTRICAL COMPONENTS
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    • B29C65/02—Joining or sealing of preformed parts, e.g. welding of plastics materials; Apparatus therefor by heating, with or without pressure
    • B29C65/18—Joining or sealing of preformed parts, e.g. welding of plastics materials; Apparatus therefor by heating, with or without pressure using heated tools
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Abstract

以低成本提供一种各向同性、外观、与金属片(4)的粘接力以及尺寸稳定性均优异的覆金属箔层叠体。包括以下两个工序：第1工序：将热塑性液晶聚合物膜和该金属片在加热辊(5，5)之间进行压接；第2工序：以热塑性液晶聚合物膜的熔点以下的加热处理温度，对在第1工序中得到的覆金属箔层叠体进行加热处理，所述热塑性液晶聚合物膜中，热塑性液晶聚合物膜(2)长度方向的热膨胀系数αL在该膜的厚度T、厚度系数β、以及各向异性系数γ的关系中，满足αL＝βT+γ公式，并且，厚度系数β在－0.08～－0.01的范围内，各向异性系数γ相对于该金属片的热膨胀系数αM，在+6～+10的范围内，且该膜的宽度方向的热膨胀系数αT相对于该金属片的热膨胀系数αM，在－2～+3的范围内。

Description

覆金属箔层叠体及其制造方法
技术领域
本发明涉及使用了由可形成光学各向异性的熔融相的热塑性聚合物(以下称为热塑性液晶聚合物)构成的膜(以下称为热塑性液晶聚合物膜)的覆金属箔层叠体及其制造方法。具体地说，本发明的覆金属箔层叠体不仅具有来自热塑性液晶聚合物膜的优异的低吸湿性、耐热性、耐化学性、以及电气性质，还具有优异的尺寸稳定性，作为柔性线路板或半导体安装用电路基板材料等是有用的。
背景技术
从移动通信开始，对携带用电子设备的小型化·轻量化的要求变高，对高密度安装的期待进一步增强。与此相伴，线路板的多层化、配线间距的窄间距化、通孔的细微化、IC包装的小型多针化在发展中，但对于电容器或电阻的无源元件，小型化和表面安装化一同在发展。特别是，将这些无源元件直接形成在印刷线路板的表面或内部的技术，以及将IC包装等的有源元件直接安装在印刷线路板表面的技术，不仅可实现高密度安装，而且可期待提高可靠性。由此，线路板的尺寸稳定性，即导体电路形成前后以及用于安装上述有源元件或无源元件的加热工序前后的尺寸变化率的要求水平变高，进而，解除其各向异性的必要性也开始提高。
另一方面，具有优异的低吸湿性、耐热性、耐化学性、以及电气特性的热塑性液晶聚合物膜，作为提高印刷线路板的可靠性的绝缘基板材料，其商品化正在急速地进行中。
以往，将热塑性液晶聚合物膜和金属片层叠制造覆金属箔层叠板，是使用真空热压装置进行的。该方法是，在2块热平盘之间放置热塑性液晶聚合物膜和金属片，在真空状态下加热压接(真空热压层叠法)。为了通过该方法获得尺寸稳定性良好的覆金属箔层叠板，需要使作为原料而使用的热塑性液晶聚合物膜的纵横的热膨胀系数接近金属片的热膨胀系数，由此，可消除尺寸稳定性的各向异性。但是，由于真空热压层叠法是薄片式的制造方法，因此需要花费材料组装时间、1次的压制时间、压制后的材料取出时间等平均1块覆金属箔层叠板的制造时间，生产速度变慢。如果要改造设备，使其能够提高生产速度，同时制造多块板的话，则设备体积变大，设备费用升高，故成本上升。因此，一直在寻求开发能解决该问题的连续的制造方法。
另一方面，为了充分发挥热塑性液晶聚合物膜的特征，进而发挥成本的优越性，则需要实现连续的与金属片的层叠，之前在各种领域进行了研究。比如，已知有用于改善与金属之间的粘结力的条件、对于改善机械强度的技术(比如，专利文献1)。而且，对于热塑性液晶聚合物膜的处理方法，特别是对于热塑性液晶聚合物膜的加热尺寸变化率的技术(比如，专利文献2)也是已知的。
专利文献1：日本特开平5-42603号文献
专利文献2：日本特开平8-90570号文献
发明内容
但是，专利文献1中没有记载有关热塑性液晶聚合物膜的尺寸稳定性的改善，专利文献2中没有记载覆金属箔层叠板的特性。而且，上述文献的技术中，难以连续稳定地获得各向同性和尺寸稳定性良好的覆金属箔层叠体。即，在加热辊之间将热塑性液晶聚合物膜与金属片压接的场合，在这些材料的卷出机与加热辊形成的空行程区间，通过至少由于自重而施加在膜长度方向(拉伸方向)的张力，以及在加热辊之间施加在膜长度方向的按压，热塑性液晶聚合物膜的分子变得容易向长度方向取向。其结果，难以得到各向同性和尺寸稳定性良好的覆金属箔层叠体。
本发明的目的在于提供一种在使用加热辊的连续制造的高生产性的前提下，各向同性、外观、与金属片的粘接力、以及尺寸稳定性优异的覆金属箔层叠体及其制造方法。
为了实现上述目的，本发明的覆金属箔层叠体的制造方法是制造一种在热塑性液晶聚合物膜的至少一个表面上接合有金属片的覆金属箔层叠体的方法，该方法包括以下两个工序，第1工序：将热塑性液晶聚合物膜和该金属片在加热辊之间进行压接；第2工序：以热塑性液晶聚合物膜的熔点以下的加热处理温度，对在第1工序中得到的覆金属箔层叠体进行加热处理，所述热塑性液晶聚合物膜中，热塑性液晶聚合物膜长度方向的热膨胀系数αL(×10-6cm/cm/℃)在该膜的厚度T(μm)、厚度系数β(×1/μm/℃)、以及各向异性系数γ(×10-6cm/cm/℃)的关系中，满足αL＝βT+γ公式，并且，厚度系数β在-0.08～-0.01的范围内(-0.08≤β≤-0.01)，各向异性系数γ相对于该金属片的热膨胀系数αM，在+6～+10(×10-6cm/cm/℃)的范围内(αM+6≤γ≤αM+10)，且该膜的宽度方向的热膨胀系数αT相对于该金属片的热膨胀系数αM，在-2～+3(×10-6cm/cm/℃)的范围内(αM-2≤αT≤αM+3)。
如上所述，在加热辊之间对超长的热塑性液晶聚合物膜与金属片进行压接时，通过这些材料中在膜长度方向施加的张力，以及在加热辊之间施加在膜长度方向的按压，在热塑性液晶聚合物膜中产生长度方向的热膨胀特性的各向异性，但在本发明中，在第1工序中，该各向异性通过使用膜的长度(纵)方向和宽度(横)方向的热膨胀系数αL、αT为特定范围的热塑性液晶聚合物膜，在连续地在膜的长度方向施加张力，在加热辊之间进行压接的场合，可通过分子在与膜的长度方向正交的方向取向的热塑性液晶聚合物膜的分子取向特性，相互抵消，可消除热塑性聚合物膜的热膨胀系数的各向异性，因此，可稳定地获得各向同性优异，外观也优异的覆金属箔层叠体。进而，通过使用该覆金属箔层叠体，在特定的温度条件下进行加热处理，与金属片的粘结力变大，可获得具有期望的尺寸变化率的尺寸稳定性优异的覆金属箔层叠体。这样，可获得在使用加热辊的连续制造的高生产性的情况下，各向同性、外观、与金属片的粘结力、以及尺寸稳定性优异的覆金属箔层叠体。
本发明使用的热塑性液晶聚合物膜的原料没有特别的限定，作为其具体实例，可列举从以下例示的分为(1)～(4)类的化合物及其衍生物导出的公知的热致液晶聚酯以及热致液晶聚酯酰胺。但是，为了得到可形成光学的各向异性的熔融相的聚合物，当然各种原料化合物的组合中具有适当的范围。
(1)芳香族或脂肪族二羟基化合物(代表例参见表1)
[表1]
Figure A20058003839500061
(2)芳香族或脂肪族二羧酸(代表例参见表2)
[表2]
(3)芳香族羟基羧酸(代表例参见表3)
[表3]
Figure A20058003839500072
(4)芳香族二胺、芳香族羟基胺或芳香族氨基羧酸(代表例参见表4)
[表4]
Figure A20058003839500073
作为由这些原料化合物得到的热塑性液晶聚合物的代表例，可列举出具有表5所示结构单位的共聚物(a)～(e)。
[表5]
Figure A20058003839500081
另外，作为本发明使用的热塑性液晶聚合物的熔点，在获得膜希望的耐热性和加工性的目的下，优选在约200℃～约400℃的范围内，特别是在约250℃～约350℃的范围内具有熔点，但从膜制造的观点来看，优选具有较低的熔点。因此，在需要更高耐热性或熔点的场合，通过对暂时获得的膜进行加热处理，可提高到希望的耐热性或熔点。对加热处理条件的一个实例进行说明，即使在暂时获得的膜的熔点为283℃的场合，如果以260℃加热5小时，则熔点变为320℃。
本发明使用的热塑性液晶聚合物膜可通过将上述热塑性液晶聚合物挤出成形而获得。此时，可使用任意的挤出成形法，但公知的T模头制膜延伸法、层压体延伸法、膨胀法等在工业上是有利的。特别是在膨胀法中，不仅是膜的机械轴方向(上述膜的长度方向)(以下省略为MD方向)，在与其正交的方向(上述膜的横向)(以下省略为TD方向)也施加应力，可得到获得了MD方向与TD方向的机械性质以及热性质的平衡的膜。
上述热塑性液晶聚合物膜中，该膜的长度方向的热膨胀系数αL(×10-6cm/cm/℃)在该膜的厚度T(μm)、厚度系数β(×1/μm/℃)、以及各向异性系数γ(×10-6cm/cm/℃)的关系中，满足αL＝βT+γ公式，并且，厚度系数β在-0.08～-0.01的范围内(-0.08≤β≤-0.01)，各向异性系数γ相对于该金属片的热膨胀系数αM，在+6～+10(×10-6cm/cm/℃)的范围内(αM+6≤γ≤αM+10)，且该膜的宽度方向的热膨胀系数αT需要相对于该金属片的热膨胀系数αM，在-2～+3(×10-6cm/cm/℃)的范围内(αM-2≤αT≤αM+3)。根据该膜的使用领域不同，必要的热膨胀系数在上述范围内也各自不同。该范围的热塑性液晶聚合物膜中，作为膜，上述MD方向与TD方向的机械性质和热性质不平衡，但不至于产生实用上的问题，如后述那样，具有可使作为覆金属箔层叠体时的各向同性、外观、与金属片的粘结力以及尺寸稳定性良好的优点。
在这里，该膜的热膨胀系数是指，以一定升温速度从室温加热到该膜的热变形温度附近时的膨胀率除以温度差得到的系数，像以下那样算出。
首先，使用公知的热机械分析装置，将切断成长条状的膜的一端固定，向另一端施加拉伸负荷，测量以一定升温速度进行加热时的膨胀量。比如，膜的拉伸负荷方向的长度为L0(mm)、加热时的膜的长度为L1(mm)、加热温度为T2(℃)、室温为T1(℃)的话，则热膨胀系数αL可通过下述式算出。
αL＝[(L1-L0)/(T2-T1)]/L0(×10-6cm/cm/℃)
本发明中，L0为20mm、T2为150℃、T1为25℃、拉伸负荷为1g。
本发明中该膜的长度(MD)方向的热膨胀系数αL(×10-6cm/cm/℃)在该膜的厚度T(μm)、厚度系数β(×1/μm/℃)、以及各向异性系数γ(×10-6cm/cm/℃)的关系中，满足αL＝βT+γ的公式。该式考虑了在膜长度方向的热膨胀系数αL中膜的厚度。
上述厚度系数β必须在-0.08～-0.01的范围内(-0.08≤β≤-0.01)。厚度系数β＞-0.01或β＜-0.08时，所得的覆金属箔层叠体的尺寸稳定性不好，MD和TD的各向异性较大。特别是在需要高尺寸稳定性的使用领域的场合，厚度系数β最好为-0.07≤β≤-0.02。
上述各向异性系数γ相对于金属片的热膨胀系数αM，必须在+6～+10(×10-6cm/cm/℃)的范围内(αM+6≤γ≤αM+10)。在γ＜αM+6或γ＞αM+10的场合，所得的覆金属箔层叠体的尺寸稳定性不好，MD和TD的各向异性较大。比如在金属片为铜箔的场合，铜的热膨胀系数为18(×10-6cm/cm/℃)，故各向异性系数γ为24≤γ≤28；在铝箔的场合，铝的热膨胀系数为23(×10-6cm/cm/℃)，故29≤γ≤33。
本发明中该膜的宽度(TD)方向的热膨胀系数αT相对于金属片的热膨胀系数αM，必须在-2～+3(×10-6cm/cm/℃)的范围内(αM-2≤αT≤αM+3)。比如在金属片为铜箔的场合，为16≤αT≤21；在铝箔的场合，为21≤αT≤26。最好，热膨胀系数αT为αM≤αT≤αM+2。
本发明的热塑性液晶聚合物膜的厚度T最好在10～250μm的范围内(10≤T≤250)。其中，作为柔性印刷线路板，使用作为电绝缘性材料而使用了热塑性液晶聚合物膜的覆金属箔层叠体的场合，其膜的膜厚优选在20～100μm的范围内，特别优选在20～50μm的范围内。膜的厚度过薄的场合，膜的刚性、强度变小，故在向所得的印刷线路板上安装电子部件时由于加压而变形，配线的位置精度变差，成为不好的原因。另外，也可在膜中混合润滑剂、抗氧化剂等添加剂或填充材料。
附图说明
通过对参考了附图的以下的优选实施例进行说明，应能更加清楚地理解本发明。但是，实施例和附图只是用于图示和说明，并不应用于限定本发明的范围。本发明的范围通过添附的权利要求书而确定。在附图中，多个附图中的同一个部件编号表示同一部分。
图1是表示实施本发明的一个实施例的覆金属箔层叠体的连续的制造方法的装置的一个实例的结构图。
图2是表示制造本发明的用于覆金属箔层叠体的热塑性液晶聚合物膜的装置的一个实例的结构图。
具体实施方式
图2表示制造热塑性液晶聚合物膜的装置的一个实例，该热塑性液晶聚合物膜是本发明的用于覆金属箔层叠体的热塑性液晶聚合物膜，上述膜的长度(纵)方向和宽度(横)方向的热膨胀系数αL、αT为特定范围。该装置在将从卷出辊11卷出的热塑性液晶聚合物膜12和从卷出辊13卷出的比如铝箔那样的支撑体14重合的状态，送入加热辊15，通过热压接而接合，制成层叠体20。
该加热辊15可以使用一对加热金属辊或一对耐热橡胶辊和加热金属辊。在图2的层叠体20的制造中，使用一对耐热橡胶辊51和加热金属辊52，在膜12侧配置有耐热橡胶辊51，在支撑体14侧配置有加热金属辊52。通过该配置，可防止膜12不必要地附着在加热金属辊52上。
然后，将层叠体20送入加热处理装置16中，在比热塑性液晶聚合物膜12的熔点低10℃的温度～比熔点高10℃的温度范围内进行加热处理。通过这样在比热塑性液晶聚合物膜12的熔点低10℃的温度～比熔点高10℃的温度范围内进行连续的加热处理，可提高热塑性液晶聚合物膜12的热膨胀系数，之后，通过上下2个剥离辊17、17将层叠体20剥离，从而使热塑性液晶聚合物膜2与支撑体14分离，可得到调整为期望的热膨胀系数的热塑性液晶聚合物膜2。这样，可得到具有上述特定范围的膜长度方向和宽度方向的热膨胀系数αL、αT的热塑性液晶聚合物膜2。加热处理装置16可以使用比如热风循环炉、热辊、陶瓷加热器等公知的机构。
图1表示实施本发明的覆金属箔层叠体的连续的制造方法的装置的一个实例。该装置在第1工序中，在将从卷出辊1卷出的具有在图2中制造的上述特定范围的膜长度方向和宽度方向的热膨胀系数αL、αT的热塑性液晶聚合物膜2，和从卷出辊3卷出的比如铜箔那样的金属片4重合的状态下，送入加热辊5中通过热压接而使其接合，制成单面的覆金属箔层叠体10。作为该加热辊5，使用一对加热金属辊或一对耐热橡胶辊和加热金属辊，该单面的覆金属箔层叠体10的制造中，与上述同样，使用一对耐热橡胶辊51和加热金属辊52。
在第1工序中，覆金属箔层叠体10在将热塑性液晶聚合物膜2和金属片4重合的状态下，在膜的长度方向施加张力，送入加热辊5，并且在加热辊51、52之间，在膜长度方向实施挤压，通过热压接使其接合，由此进行层叠。此时的热塑性液晶聚合物膜2上产生的朝向膜长度方向的热膨胀系数的各向异性，通过使用具有上述特定范围的膜长度方向和宽度方向的热膨胀系数αL、αT的热塑性液晶聚合物膜2，在连续地在膜长度方向施加张力，在加热辊51、52之间压接的场合，由于在与膜长度方向正交的方向上分子取向的热塑性液晶聚合物膜2的分子取向特性而抵消。这样，热塑性聚合物膜2的热膨胀系数的各向异性被解除，故可稳定地得到各向同性优异，外观也优异的覆金属箔层叠体10。
该装置在第2工序中，将在第1工序中得到的覆金属箔层叠体10送入加热处理装置6中，以热塑性液晶聚合物膜2的熔点以下的加热处理温度进行加热处理。由此，与金属片4的粘接力大，可得到具有期望的尺寸变化率的尺寸稳定性优异的覆金属箔层叠体10。为了进一步增大与金属片4的粘接力，加热处理温度优选在比该膜2的熔点低5℃～20℃的温度范围。在加热处理温度为超过熔点的温度的场合，会产生发泡现象或显著的热膨胀系数的变化，有无法得到规定的品质的情况。在加热处理温度为比熔点低20℃的温度以下的场合，无助于与金属片4的粘接力的增加，根据金属片4的种类，有无法达到要求的粘接力的情况。作为加热处理装置6，与上述同样，可使用热风循环炉、热辊、陶瓷加热器等。在经过该第2工序后，通过卷绕辊7将覆金属箔层叠体10卷绕成辊状。
以下，通过实施例对本发明进行详细的说明，但本发明并不受这些实施例的任何限定。另外，在以下的实施例中，热塑性液晶聚合物膜的熔点、层叠体的粘接强度以及尺寸稳定性通过以下的方法测定。
(1)熔点
使用差示扫描热量计观察并获得膜的热特性。即，以20℃/分的速度使试验膜升温，使其完全熔融后，以50℃/分的速度使熔融物骤冷到50℃，再以20℃/分的速度升温，将此时展现的吸热峰值的位置作为膜的熔点而记录。
(2)粘接强度
由层叠体制作1.5cm宽的剥离试验片，将该膜层用双面粘接带固定在平板上，以JIS C5016为准，通过180°法以50mm/分的速度将金属箔剥离，测定出此时的粘接强度(Kg/cm)。
(3)尺寸稳定性
尺寸稳定性以IPC-TM-6502.2.4为准进行了测定。
参考例1
用对羟基苯甲酸和6-羟基-2-萘酸的共聚物，熔融挤出熔点为280℃的液晶聚合物，一边控制纵横的延伸比，一边通过膨胀成形法得到膜厚为25、50、100以及225μm的膜，与涂敷了脱模剂的30μm厚的铝箔重合，在260℃的加热金属辊与耐热橡胶辊之间以20kg/cm2进行热压接后，在设定好温度的热处理炉中进行30秒热处理，以使各膜厚的膜的MD方向的热膨胀系数αL成为下述规定值。接着，在氮气氛下的烘箱中，在260℃下进行6小时热处理，然后，将铝箔剥离，得到熔点为305℃，TD方向的热膨胀系数αT在全部厚度上为19×10-6cm/cm/℃，MD方向的热膨胀系数αL各自的厚度为25.3、24.5、23以及19.3×10-6cm/cm/℃(β＝-0.03，γ＝26)的膜。将这些热塑性液晶聚合物膜作为A。
在参考例1中，比如，在层叠热塑性液晶聚合物膜A和铜箔(金属片)的场合，膜的厚度T为25、50、100、225μm，故满足10≤T≤250；厚度系数β为-0.03，故满足-0.08≤β≤-0.01；各向异性系数γ为26，故铜箔的热膨胀系数αM为18×10-6cm/cm/℃，满足αM+6≤γ≤αM+10。热膨胀系数αT在全部厚度上为19×10-6cm/cm/℃，故满足αM-2≤αT≤αM+3。热膨胀系数αL与在αL＝βT+γ的公式中代入了各厚度T、厚度系数β、各向异性系数γ的值一致。即，热塑性液晶聚合物膜A的各数值包含在本发明的范围内。
参考例2
用对羟基苯甲酸和6-羟基-2-萘酸的共聚物，熔融挤出熔点为280℃的液晶聚合物，一边控制纵横的延伸比，一边通过膨胀成形法得到膜厚为25、50、100以及225μm的膜，与涂敷了脱模剂的30μm厚的铝箔重合，在260℃的加热辊与耐热橡胶辊之间以20kg/cm2进行热压接后，在设定好温度的热处理炉中进行30秒热处理，以使各膜厚的膜的MD方向的热膨胀系数αL成为下述规定值。接着，在氮气氛下的烘箱中，在260℃下进行6小时热处理，然后，将铝箔剥离，得到熔点为305℃，TD方向的热膨胀系数αT在全部厚度上为19×10-6cm/cm/℃，MD方向的热膨胀系数αL各自的厚度为23.5、23、22以及19.5×10-6cm/cm/℃(β＝-0.02，γ＝24)的膜。将这些热塑性液晶聚合物膜作为B。
在参考例2中，与参考例1同样地层叠热塑性液晶聚合物膜B和铜箔(金属片)的场合，膜的厚度T同样地满足，厚度系数β为-0.02，故满足-0.08≤β≤-0.01；各向异性系数γ为24，故铜箔的热膨胀系数αM为18×10-6cm/cm/℃，满足αM+6≤γ≤αM+10。热膨胀系数αT在全部厚度上为19×10-6cm/cm/℃，故满足αM-2≤αT≤αM+3。热膨胀系数αL同样与在αL＝βT+γ的公式中代入了各数值的值一致。即，热塑性液晶聚合物膜B的各数值包含在本发明的范围内。
参考例3
用对羟基苯甲酸和6-羟基-2-萘酸的共聚物，熔融挤出熔点为280℃的液晶聚合物，一边控制纵横的延伸比，一边通过膨胀成形法得到膜厚为25、50、100以及225μm的膜，与涂敷了脱模剂的30μm厚的铝箔重合，在260℃的加热辊与耐热橡胶辊之间以20kg/cm2进行热压接后，在设定好温度的热处理炉中进行30秒热处理，以使各膜厚的膜的MD方向的热膨胀系数αL成为下述规定值。接着，在氮气氛下的烘箱中，在260℃下进行6小时热处理，然后，将铝箔剥离，得到熔点为305℃，TD、MD方向的热膨胀系数αT、热膨胀系数αL在全部厚度上为18×10-6cm/cm/℃(β＝0，γ＝18)的膜。将这些热塑性液晶聚合物膜作为C。
在参考例3中，与参考例1同样地层叠热塑性液晶聚合物膜C和铜箔(金属片)的场合，膜的厚度T同样地满足，厚度系数β为0，故不满足-0.08≤β≤-0.01；各向异性系数γ为18，故铜箔的热膨胀系数αM为18×10-6cm/cm/℃，不满足αM+6≤γ≤αM+10。热膨胀系数αT在全部厚度上为18×10-6cm/cm/℃，故满足αM-2≤αT≤αM+3。热膨胀系数αL同样与在αL＝βT+γ的公式中代入了各数值的值一致。即，热塑性液晶聚合物膜C的厚度系数β和各向异性系数γ不包含在本发明的范围内。
参考例4
用对羟基苯甲酸和6-羟基-2-萘酸的共聚物，熔融挤出熔点为280℃的液晶聚合物，一边控制纵横的延伸比，一边通过膨胀成形法得到膜厚为25、50、100以及225μm的膜，与涂敷了脱模剂的30μm厚的铝箔重合，在260℃的加热辊与耐热橡胶辊之间以20kg/cm2进行热压接后，在设定好温度的热处理炉中进行30秒热处理，以使各膜厚的膜的MD方向的热膨胀系数αL成为下述规定值。接着，在氮气氛下的烘箱中，在260℃下进行6小时热处理，然后，将铝箔剥离，得到熔点为305℃，TD方向的热膨胀系数αT在全部厚度上为19×10-6cm/cm/℃，MD方向的热膨胀系数αL各自的厚度为16.5、15、12、4.5×10-6cm/cm/℃(β＝-0.06，γ＝18)的膜。将这些热塑性液晶聚合物膜作为D。
在参考例4中，与参考例1同样地层叠热塑性液晶聚合物膜D和铜箔(金属片)的场合，膜的厚度T同样地满足，厚度系数β为-0.06，故满足-0.08≤β≤-0.01；各向异性系数γ为18，故铜箔的热膨胀系数αM为18×10-6cm/cm/℃，不满足αM+6≤γ≤αM+10。热膨胀系数αT在全部厚度上为19×10-6cm/cm/℃，故满足αM-2≤αT≤αM+3。热膨胀系数αL同样与在αL＝βT+γ的公式中代入了各数值的值一致。即，热塑性液晶聚合物膜D的各向异性系数γ不包含在本发明的范围内。
实施例1
使用在参考例1中得到的热塑性液晶聚合物膜A和厚度为18μm的电解铜箔(热膨胀系数18×10-6cm/cm/℃)。并且，在连续热辊压装置中安装耐热橡胶辊(硬度90度)和加热金属辊，在将热塑性液晶聚合物膜A和铜箔导入加热辊中的空行程区间中，在400mm的宽度上施加2kg的张力，供给到加热辊之间，在300℃的加热状态下以20Kg/cm2进行压接，制作热塑性液晶聚合物膜/电解铜箔的结构的层叠体。接着，导入270℃的氮气氛下的烘箱中进行30秒热处理。对所得的层叠体的粘接强度和尺寸稳定性进行试验，结果示于表6中。如表6所示，可得到粘接强度和尺寸稳定性优异的覆金属箔层叠体。
实施例2
除了使用在参考例2中获得的热塑性液晶聚合物膜B以外，与实施例1同样地层叠，对所得的覆金属箔层叠体的粘接强度和尺寸稳定性进行试验，结果示于表6中。如表6所示，可得到粘接强度和尺寸稳定性优异的覆金属箔层叠体。
比较例1
除了使用在参考例3中获得的热塑性液晶聚合物膜C以外，与实施例1同样地操作，对所得的覆金属箔层叠体的粘接强度和尺寸稳定性进行试验，结果示于表6中。如表6所示，该覆金属箔层叠体MD方向的尺寸稳定性不好。
比较例2
除了使用在参考例4中获得的热塑性液晶聚合物膜D以外，与实施例1同样地操作，对所得的覆金属箔层叠体的粘接强度和尺寸稳定性进行试验，结果示于表6中。如表6所示，该覆金属箔层叠体MD方向的尺寸稳定性不好。
比较例3
使用在参考例1中得到的热塑性液晶聚合物膜A和厚度为18μm的电解铜箔(热膨胀系数18×10-6cm/cm/℃)。并且，在连续热辊压装置中安装耐热橡胶辊(硬度90度)和加热金属辊，在将液晶聚合物膜A和铜箔导入加热辊中的空行程区间中，在400mm的宽度上施加2kg的张力，供给到加热辊之间，在300℃的加热状态下以20Kg/cm2进行压接，制作热塑性液晶聚合物膜/电解铜箔的结构的层叠体。对所得的覆金属箔层叠体的粘接强度和尺寸稳定性进行试验，结果示于表6中。如表6所示，该覆金属箔层叠体由于是通过不包含本发明第2工序的制造方法制作的，故粘接强度不好。
[表6]
厚度系数β   各向异性系数γ   粘接强度(kg/cm)       尺寸稳定性(％)
  MD方向   TD方向
 实施例1   -0.03   26   1.2   -0.01   +0.01
 实施例2   -0.02   24   1.3   +0.01   +0.01
 比较例1   0   18   1.0   +0.25   +0.01
 比较例2   -0.06   18   1.2   +0.20   +0.01
 比较例3   -0.03   26   0.7   -0.01   +0.01

Claims (5)

1.一种覆金属箔层叠体的制造方法，所述覆金属箔层叠体在膜的至少一个表面上接合有金属片，所述膜由可形成光学各向异性的熔融相的热塑性聚合物构成(以下将其称为热塑性液晶聚合物膜)，该覆金属箔层叠体的制造方法的特征在于，
包括以下两个工序，第1工序：将热塑性液晶聚合物膜和该金属片在加热辊之间进行压接；第2工序：以热塑性液晶聚合物膜的熔点以下的加热处理温度，对在第1工序中得到的覆金属箔层叠体进行加热处理，所述热塑性液晶聚合物膜中，热塑性液晶聚合物膜长度方向的热膨胀系数αL(×10-6cm/cm/℃)在该膜的厚度T(μm)、厚度系数β(×1/μm/℃)、以及各向异性系数γ(×10-6cm/cm/℃)的关系中，满足αL＝βT+γ公式，并且，厚度系数β在-0.08～-0.01的范围内，各向异性系数γ相对于该金属片的热膨胀系数αM，在+6～+10(×10-6cm/cm/℃)的范围内，且该膜的宽度方向的热膨胀系数αT相对于该金属片的热膨胀系数αM，在-2～+3(×10-6cm/cm/℃)的范围内。
2.根据权利要求1记载的覆金属箔层叠体的制造方法，其特征在于，热塑性液晶聚合物膜的厚度T为10～250μm的范围。
3.根据权利要求1记载的覆金属箔层叠体的制造方法，其特征在于，所述覆金属箔层叠体是在热塑性液晶聚合物膜的两个表面上结合了金属片的双面覆金属箔层叠体。
4.根据权利要求1记载的覆金属箔层叠体的制造方法，其特征在于，第2工序的加热处理温度为比该膜的熔点低5℃～20℃的温度范围。
5.一种覆金属箔层叠体，其特征在于，其通过权利要求1记载的制造方法制造。
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