TW201819179A - 撓性金屬貼合積層板之製造方法 - Google Patents

撓性金屬貼合積層板之製造方法 Download PDF

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Publication number
TW201819179A
TW201819179A TW106118211A TW106118211A TW201819179A TW 201819179 A TW201819179 A TW 201819179A TW 106118211 A TW106118211 A TW 106118211A TW 106118211 A TW106118211 A TW 106118211A TW 201819179 A TW201819179 A TW 201819179A
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Taiwan
Prior art keywords
laminated
thermoplastic
manufacturing
thermoplastic polyimide
layer
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TW106118211A
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English (en)
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TWI784955B (zh
Inventor
間山孝之
鈴木直樹
三輪卓
藤田秀一
中村健二
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有澤製作所股份有限公司
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    • 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
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    • 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
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    • B32B15/088—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 comprising polyamides
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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
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    • B29C65/00—Joining or sealing of preformed parts, e.g. welding of plastics materials; Apparatus therefor
    • B29C65/48—Joining or sealing of preformed parts, e.g. welding of plastics materials; Apparatus therefor using adhesives, i.e. using supplementary joining material; solvent bonding
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    • B29C66/90—Measuring or controlling the joining process
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    • 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
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    • B29C66/91943—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 Tg, i.e. the glass transition temperature, of the material of one of the parts to be joined higher than said glass transition temperature
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
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Abstract

本發明之撓性金屬貼合積層板之製造方法包括以下步驟： (a)藉由聚醯亞胺樹脂膜與金屬箔貼合，獲得積層體，上述聚醯亞胺樹脂膜包含非熱塑性聚醯亞胺層、及含有熱塑性聚醯亞胺之接著層，且於上述非熱塑性聚醯亞胺層之至少單面設有上述接著層；及 (b)將上述步驟(a)中所獲得之積層體於惰性氣體氛圍、且0.20～0.98 Mpa之壓力下，以上述熱塑性聚醯亞胺之Tg-20℃～Tg+50℃之溫度進行熱處理。

Description

撓性金屬貼合積層板之製造方法
本發明係關於一種撓性金屬貼合積層板之製造方法。
先前，於電子材料領域，使用有將具有電絕緣性之聚醯亞胺膜或聚醯胺膜等樹脂層、以環氧樹脂或聚醯亞胺樹脂為主成分之接著劑層、具有導電性之銅箔、銀箔、鋁箔等金屬箔層等適宜組合而成之覆蓋層或撓性金屬貼合積層板等撓性印刷配線板(FPC)用材料。作為撓性金屬貼合積層板，主要已知有包含金屬層、及聚醯亞胺樹脂層之2層撓性金屬貼合積層板；及包含金屬層、聚醯亞胺樹脂層、及接著層之3層撓性金屬積層板。 近年來，為了達成電子機器之進一步小型化、輕量化，設置於基板之配線之微細化不斷推進，要安裝之零件亦搭載小型化、高密度化之零件。因此，若於微細配線形成之後產生較大之尺寸變化，有可能會產生零件之搭載位置偏離設計階段之位置，零件與基板變得不再良好地連接之問題。一直以來，作為抑制尺寸變化之嘗試，進行有控制層壓壓力，或控制接著膜之張力等。然而，雖然該等手段雖使尺寸變化得到一定程度之改善，但仍不夠充分，要求進一步抑制尺寸變化。 作為解決上述問題點之手段，專利文獻1中揭示藉由於層壓後將保護材料與撓性金屬貼合積層板密接之積層體以在MD方向上施加特定之張力的狀態下搬送，可抑制尺寸變化。 又，專利文獻2中揭示藉由將於玻璃轉移區域所觀察到之吸熱波峰之熱量調節至特定範圍，可減小由撓性金屬箔積層體之熱縮導致之尺寸變化率及其偏差，且記載有此種積層體係藉由以較樹脂之玻璃轉移點Tg低5～50℃之溫度進行8小時以上之熱處理而獲得。 先前技術文獻 專利文獻 專利文獻1：日本專利特開2015-51636號公報 專利文獻2：日本專利特開2005-119178號公報
[發明所欲解決之問題] 然而，專利文獻1之撓性金屬貼合積層板雖然某個特定區域之尺寸變化得到抑制，但尺寸變化率有偏差，不可謂尺寸變化於積層板整體上得到均一抑制。 又，專利文獻2之撓性印刷金屬箔積層體需要8小時以上之長時間之熱處理，生產性欠佳。又，假設於為了縮短熱處理之時間而以更高溫進行熱處理之情形時，會產生因積層體中所含之空氣膨脹導致表面發生鼓出，外觀欠佳之類的問題。 鑒於上述情況，本發明之目的在於提供一種可效率良好地生產尺寸變化於積層板整體上得到均一抑制、且表面無鼓出之撓性金屬貼合積層板的撓性金屬貼合積層板之製造方法。 [解決問題之技術手段] 本發明者等人為了解決上述問題進行了銳意研討，結果發現藉由於將在非熱塑性聚醯亞胺層之至少單面設置含有熱塑性聚醯亞胺之接著層之聚醯亞胺樹脂膜、與金屬箔貼合後，將所獲得之積層體於惰性氣體氛圍、且0.20～0.98 MPa之壓力下，以上述熱塑性聚醯亞胺之Tg-20℃～Tg+50℃之溫度進行熱處理，可解決上述問題，從而完成了本發明。 即，本發明如下所述。 [1] 一種撓性金屬貼合積層板之製造方法，其包括以下步驟： (a)藉由將聚醯亞胺樹脂膜與金屬箔貼合，獲得積層體，上述聚醯亞胺樹脂膜包含非熱塑性聚醯亞胺層、及含有熱塑性聚醯亞胺之接著層，且於上述非熱塑性聚醯亞胺層之至少單面設有上述接著層；及 (b)將上述步驟(a)中所獲得之積層體於惰性氣體氛圍、且0.20～0.98 Mpa之壓力下，以上述熱塑性聚醯亞胺之Tg-20℃～Tg+50℃之溫度進行熱處理。 [2] 如上述[1]所記載之製造方法，其中於上述步驟(a)中，聚醯亞胺樹脂膜與金屬箔係藉由層壓而貼合。 [3] 如上述[1]或[2]所記載之製造方法，其中於上述步驟(b)中，以上述熱塑性聚醯亞胺之Tg-10℃～Tg+30℃之溫度進行熱處理。 [4] 如上述[1]～[3]中任一項所記載之製造方法，其中上述步驟(b)中之熱處理時間為60～420分鐘。 [5] 如上述[1]～[4]中任一項所記載之製造方法，其中於上述步驟(b)中，積層體為捲筒狀。 [6] 如上述[1]～[5]中任一項所記載之製造方法，其係於高壓釜內進行上述步驟(b)。 [7] 如上述[1]～[6]中所記載之製造方法，其中上述熱塑性聚醯亞胺之Tg為240～290℃。 [8] 如上述[1]～[7]中任一項所記載之製造方法，其中上述撓性金屬貼合積層板為單面金屬貼合積層板。 [9] 如上述[1]～[7]中任一項所記載之製造方法，其中上述撓性金屬貼合積層板為雙面金屬貼合積層板。 [發明之效果] 根據本發明之製造方法，可於短時間內效率良好地生產尺寸變化於積層板整體上得到均一抑制、且表面無鼓出之撓性金屬貼合積層板。
以下，對用於實施本發明之形態(以下，稱為「本實施形態」)進行詳細記載。再者，本發明並不限定於以下之實施形態，可於其主旨之範圍內進行各種變化而實施。 本實施形態中之撓性金屬貼合積層板之製造方法 係撓性金屬貼合積層板之製造方法，其包括以下步驟： (a)藉由將聚醯亞胺樹脂膜與金屬箔貼合，獲得積層體，上述聚醯亞胺樹脂膜包含非熱塑性聚醯亞胺層、及含有熱塑性聚醯亞胺之接著層，且於上述非熱塑性聚醯亞胺層之至少單面設有上述接著層；及 (b)將上述步驟(a)中所獲得之積層體於惰性氣體氛圍、且0.20～0.98 Mpa之壓力下，以上述熱塑性聚醯亞胺之Tg-20℃～Tg+50℃之溫度進行熱處理。 以下，亦將上述步驟(a)及步驟(b)分別稱為「積層步驟」及「熱處理步驟」。 [步驟(a)] 本實施形態之製造方法中之步驟(a)係以下步驟：藉由將聚醯亞胺樹脂膜與金屬箔貼合，獲得積層體，上述聚醯亞胺樹脂膜包含非熱塑性聚醯亞胺層、及含有熱塑性聚醯亞胺之接著層，且於上述非熱塑性聚醯亞胺層之至少單面設有上述接著層。 非熱塑性聚醯亞胺層中所用之非熱塑性聚醯亞胺例如藉由將酸二酐與二胺共聚而獲得。作為酸二酐及二胺，可使用脂肪族化合物、脂環式化合物、芳香族化合物之任一者，但就耐熱性之觀點而言，作為酸二酐，較佳為芳香族四羧酸二酐；作為二胺，較佳為芳香族二胺。 作為構成非熱塑性聚醯亞胺之酸二酐，例如可列舉選自由焦蜜石酸二酐、2,3,6,7-萘四羧酸二酐、3,3',4,4'-聯苯四羧酸二酐、1,2,5,6-萘四羧酸二酐、2,2',3,3'-聯苯四羧酸二酐、3,3',4,4'-二苯甲酮四羧酸二酐、4,4'-氧二鄰苯二甲酸二酐、2,2-雙(3,4-二羧基苯基)丙烷二酐、3,4,9,10-二萘嵌苯四羧酸二酐、雙(3,4-二羧基苯基)丙烷二酐、1,1-雙(2,3-二羧基苯基)乙烷二酐、1,1-雙(3,4-二羧基苯基)乙烷二酐、雙(2,3-二羧基苯基)甲烷二酐、雙(3,4-二羧基苯基)乙烷二酐、雙(3,4-二羧基苯基)碸二酐、對伸苯基雙(偏苯三甲酸單酯酸酐)、伸乙基雙(偏苯三甲酸單酯酸酐)、雙酚A雙(偏苯三甲酸單酯酸酐)所組成之群中之至少1種酸二酐，上述中，就耐熱性、尺寸穩定性之觀點而言，較佳為選自由焦蜜石酸二酐、2,3,6,7-萘四羧酸二酐、2,2',3,3'-聯苯四羧酸二酐、3,3',4,4'-聯苯四羧酸二酐、3,3',4,4'-二苯甲酮四羧酸二酐所組成之群中之至少1種酸二酐。 作為構成非熱塑性聚醯亞胺之二胺，例如可列舉選自由4,4'-二胺基二苯丙烷、4,4'-二胺基二苯甲烷、聯苯胺、3,3'-二氯聯苯胺、3,3'-二甲基聯苯胺、2,2'-二甲基聯苯胺、3,3'-二甲氧基聯苯胺、2,2'-二甲氧基聯苯胺、4,4'-二胺基二苯硫醚、3,3'-二胺基二苯基碸、4,4'-二胺基二苯基碸、4,4'-二胺基二苯醚、3,3'-二胺基二苯醚、3,4'-二胺基二苯醚、1,5-二胺基萘、2,6-二胺基萘、4,4'-二胺基二苯基二乙基矽烷、4,4'-二胺基二苯基矽烷、4,4'-二胺基二苯基乙基氧化膦、4,4'-二胺基二苯基N-甲基胺、4,4'-二胺基二苯基N-苯胺、1,4-二胺基苯(對伸苯基二胺)、1,3-二胺基苯、1,2-二胺基苯、雙{4-(4-胺基苯氧基)苯基}碸、雙{4-(3-胺基苯氧基)苯基}碸、4,4'-雙(4-胺基苯氧基)聯苯、4,4'-雙(3-胺基苯氧基)聯苯、1,3-雙(3-胺基苯氧基)苯、1,3-雙(4-胺基苯氧基)苯、1,4-雙(4-胺基苯氧基)苯、3,3'-二胺基二苯甲酮、4,4'-二胺基二苯甲酮、2,2-雙[4-(4-胺基苯氧基)苯基)]丙烷所組成之群中之至少1種二胺，上述中，就耐熱性、尺寸穩定性之觀點而言，較佳為含有選自由3,3'-二甲基聯苯胺、2,2'-二甲基聯苯胺、3,3'-二甲氧基聯苯胺、2,2'-二甲氧基聯苯胺、1,5-二胺基萘、1,4-二胺基苯(對伸苯基二胺)所組成之群中之至少1種二胺。 非熱塑性聚醯亞胺之玻璃轉移溫度(Tg)由於取決於撓性金屬貼合積層板之用途，故而無特別限定，較佳為290℃以上，更佳為320℃以上，進而較佳為340℃以上。若非熱塑性聚醯亞胺之Tg為290℃以上，則有耐熱性變得良好之傾向。 再者，於本說明書中，玻璃轉移溫度(Tg)可基於利用動態黏彈性測定裝置(DMA)而測定之儲存模數之彎曲點之值而求出，具體而言，可根據後述之實施例之方法測定。 本實施形態中之接著層係設於非熱塑性聚醯亞胺層之至少單面、且含有熱塑性聚醯亞胺之層。作為接著層所用之熱塑性聚醯亞胺，可列舉熱塑性聚醯亞胺、熱塑性聚醯胺醯亞胺、熱塑性聚醚醯亞胺、熱塑性聚酯醯亞胺等。其中，就低吸濕特性之觀點而言，較佳為熱塑性聚酯醯亞胺。熱塑性聚醯亞胺例如可藉由將酸二酐與二胺共聚而獲得。 作為構成熱塑性聚醯亞胺之酸二酐，例如可列舉選自由焦蜜石酸二酐、2,3,6,7-萘四羧酸二酐、3,3',4,4'-聯苯四羧酸二酐、1,2,5,6-萘四羧酸二酐、2,2',3,3'-聯苯四羧酸二酐、3,3',4,4'-二苯甲酮四羧酸二酐、4,4'-氧二鄰苯二甲酸二酐、2,2-雙(3,4-二羧基苯基)丙烷二酐、3,4,9,10-二萘嵌苯四羧酸二酐、2,2-雙(3,4-二羧基苯基)丙烷二酐、1,1-雙(2,3-二羧基苯基)乙烷二酐、1,1-雙(3,4-二羧基苯基)乙烷二酐、雙(2,3-二羧基苯基)甲烷二酐、1,2-雙(3,4-二羧基苯基)乙烷二酐、雙(3,4-二羧基苯基)碸二酐、對伸苯基雙(偏苯三甲酸單酯酸酐)、伸乙基雙(偏苯三甲酸單酯酸酐)、雙酚A雙(偏苯三甲酸單酯酸酐)所組成之群中之至少1種，上述中，就接著性、獲得容易性之觀點而言，較佳為選自由2,2',3,3'-聯苯四羧酸二酐、3,3',4,4'-聯苯四羧酸二酐、3,3',4,4'-二苯甲酮四羧酸二酐、4,4'-氧二鄰苯二甲酸二酐所組成之群中之至少1種。 作為構成熱塑性聚醯亞胺之二胺，例如可列舉選自由4,4'-二胺基二苯丙烷、4,4'-二胺基二苯甲烷、聯苯胺、3,3'-二氯聯苯胺、3,3'-二甲基聯苯胺、2,2'-二甲基聯苯胺、3,3'-二甲氧基聯苯胺、2,2'-二甲氧基聯苯胺、4,4'-二胺基二苯硫醚、3,3'-二胺基二苯基碸、4,4'-二胺基二苯基碸、4,4'-二胺基二苯醚、3,3'-二胺基二苯醚、3,4'-二胺基二苯醚、1,5-二胺基萘、2,6-二胺基萘、4,4'-二胺基二苯基二乙基矽烷、4,4'-二胺基二苯基矽烷、4,4'-二胺基二苯基乙基氧化膦、4,4'-二胺基二苯基N-甲基胺、4,4'-二胺基二苯基N-苯胺、1,4-二胺基苯(對伸苯基二胺)、1,3-二胺基苯、1,2-二胺基苯、雙{4-(4-胺基苯氧基)苯基}碸、雙{4-(3-胺基苯氧基)苯基}碸、4,4'-雙(4-胺基苯氧基)聯苯、4,4'-雙(3-胺基苯氧基)聯苯、1,3-雙(3-胺基苯氧基)苯、1,3-雙(4-胺基苯氧基)苯、1,4-雙(4-胺基苯氧基)苯、1,3-雙(3-胺基苯氧基)苯、3,3'-二胺基二苯甲酮、4,4'-二胺基二苯甲酮、2,2-雙[4-(4-胺基苯氧基)苯基]丙烷所組成之群中之至少1種，上述中，就接著性、獲得容易性之觀點而言，較佳為選自由2,2-雙-[4-(4-胺基苯氧基)苯基]丙烷、4,4'-二胺基二苯醚、4,4'-二胺基二苯甲烷、1,3-雙(3-胺基苯氧基)苯、1,3-雙(4-胺基苯氧基)苯所組成之群中之至少1種。 熱塑性聚醯亞胺之Tg由於取決於撓性金屬貼合積層板之用途，故而無特別限定，較佳為240～290℃，更佳為260～290℃，進而較佳為280～290℃。若熱塑性聚醯亞胺之Tg為240℃以上，則有耐熱性變得良好之傾向，若為290℃以下，則有與金屬箔之貼合變得容易之傾向。 包含非熱塑性聚醯亞胺層、及含有熱塑性聚醯亞胺之接著層的聚醯亞胺樹脂膜之厚度由於取決於撓性金屬貼合積層板之用途，故而無特別限定，較佳為12.5～50 μm，更佳為12.5～25 μm。若聚醯亞胺樹脂膜之厚度未達12.5 μm，則有絕緣性欠佳之傾向，又有撕裂、破損等機械特性變低之傾向。另一方面，若聚醯亞胺樹脂膜之厚度超過50 μm，則有變得容易於熱處理時產生發泡、或柔軟性受損之傾向。 作為聚醯亞胺樹脂膜，亦可使用市售品，適宜市售品例如可列舉Kaneka公司製造之商品名「Pixeo FRS」系列、「Pixeo FC」系列、或宇部興產公司製造之商品名「Upilex NVT」系列等。 作為本實施形態中之金屬箔，並無特別限定，可列舉電解銅箔、壓延銅箔、鋁箔、不鏽鋼箔等，其中，就導電性、電路加工性之觀點而言，較佳為電解銅箔、壓延銅箔。金屬箔之厚度由於取決於撓性金屬貼合積層板之用途，故而無特別限定，較佳為1～35 μm，更佳為9～18 μm。若金屬箔之厚度未達1 μm，則有變得容易在製作電路基板時因針孔或破損等引起電路缺損之傾向，若超過35 μm，則有與聚醯亞胺樹脂膜之貼合溫度變高而生產性降低之傾向。又，金屬箔之表面亦可實施利用鍍鋅、鍍鉻等進行之無機表面處理、利用矽烷偶合劑等進行之有機表面處理。 作為金屬箔，亦可使用市售品，適宜市售品例如可列舉JX金屬公司製造之商品名「壓延銅箔BHY」、福田金屬公司製造之商品名「壓延銅箔ROFL」等。 於積層步驟中，於非熱塑性聚醯亞胺層之單面或雙面經由含有熱塑性聚醯亞胺之接著層而貼合金屬箔。作為貼合之順序，例如可列舉如下方法等：(i)於在非熱塑性聚醯亞胺層之至少單面形成接著層而獲得聚醯亞胺樹脂膜後，與金屬箔貼合；(ii)於將接著層片狀成形，且將其貼合於非熱塑性聚醯亞胺層而獲得聚醯亞胺樹脂膜後，與金屬箔貼合；(iii)將接著層片狀成形，且夾持於金屬箔與非熱塑性聚醯亞胺層之間而貼合。 於上述(i)方法之情形時，聚醯亞胺樹脂膜例如可藉由如下方式而獲得，即於非熱塑性聚醯亞胺層之至少單面塗佈作為熱塑性聚醯亞胺之前驅物的聚醯胺酸溶液並進行加熱乾燥使之醯亞胺化。 對於非熱塑性聚醯亞胺層，亦可視需要於設置接著層之前實施電暈處理、電漿處理、偶合處理等各種表面處理。又，非熱塑性聚醯亞胺層及接著層亦可含有1種以上之有機或無機填料等其他成分。 於積層步驟中，作為將聚醯亞胺樹脂膜與金屬箔貼合之方法，可使用壓製、層壓等，但就捲筒化或生產性之觀點而言，較佳為使用層壓。層壓例如可藉由具有一對以上之金屬輥之熱輥層壓裝置或雙帶式壓製機(DBP)進行，其中，熱輥層壓裝置具有構成簡單且於維護成本方面有利之優點。此處所謂之「具有一對以上之金屬輥之熱輥層壓裝置」係只要為具有用於對材料進行加熱加壓之金屬輥的裝置即可，其具體之裝置構成無特別限定。 又，亦可設置於積層步驟之前進給被積層材料之進給裝置，亦可設置於積層步驟之後捲取被積層材料之捲取裝置。藉由設置該等裝置，可更進一步地提高撓性金屬貼合積層板之生產性。進給裝置及捲取裝置之具體構成無特別限定，例如可列舉能夠捲取聚醯亞胺樹脂膜或金屬箔、或者所獲得之積層體的公知之捲筒狀捲取機等。 藉由層壓進行積層步驟之情形時之層壓溫度較佳為熱塑性聚醯亞胺樹脂之Tg+50℃以上之溫度，更佳為Tg+70℃以上。於為Tg+50℃以上之溫度之情形時，有聚醯亞胺樹脂膜與金屬箔之接著性變得良好之傾向，於為Tg+70℃以上之溫度之情形時，有可提昇層壓速度而進一步提高其生產性之傾向。作為層壓溫度之上限，無特別限定，若過高則有樹脂分解之虞。 層壓中之層壓速度較佳為0.5 m/分鐘以上，更佳為1.0 m/分鐘以上。於為0.5 m/分鐘以上之情形時，有接著性變得良好之傾向，於為1.0 m/分鐘以上之情形時，有生產性更進一步提高之傾向。 層壓壓力有越高則可越降低層壓溫度且加速層壓速度之優點，但一般若層壓壓力過高，則有所獲得之金屬貼合積層板之尺寸變化發生變差之傾向。又，反之，若層壓壓力過低，則有所獲得之積層板之接著性欠佳之傾向。因此，層壓壓力較佳為500 kg/m～5000 kg/m之範圍內，更佳為1000 kg/m～3000 kg/m之範圍內。此處，所謂層壓壓力意指金屬輥施加至材料之壓力。 層壓時之聚醯亞胺樹脂膜張力較佳為0.1～20 kg/m，更佳為0.2～15 kg/m，進而較佳為0.5～10 kg/m。若張力未達0.1 kg/m，則有變得難以獲得外觀良好之撓性金屬貼合積層板之傾向，若超過20 kg/m，則有尺寸穩定性欠佳之傾向。此處，所謂聚醯亞胺樹脂膜張力係指施加至層壓前之聚醯亞胺樹脂膜之張力。 [步驟(b)] 本實施形態中之步驟(b)係以下步驟，即將上述步驟(a)中所獲得之積層體於惰性氣體氛圍、且0.20～0.98 MPa之壓力下，以上述熱塑性聚醯亞胺之Tg-20℃～Tg+50℃之溫度進行熱處理。 步驟(b)中之熱處理係於惰性氣體氛圍、且0.20～0.98 MPa之壓力下進行。先前，已知將積層有銅箔與成為基材之樹脂的銅貼合積層板於氮氣等惰性氣體氛圍下進行熱處理，但於在較樹脂之Tg附近高之溫度下進行熱處理之情形時，積層體中所含之空氣發生膨脹而於表面產生鼓出，又，有樹脂發生熱分解之風險。因此，例如，如專利文獻2中所記載般，必須於較樹脂之Tg低之溫度下進行長時間熱處理，不可謂撓性金屬貼合積層板之生產性良好。 本發明者等人發現：藉由於金屬箔與基材樹脂之間設置含有熱塑性聚醯亞胺之接著層，且將所獲得之積層體於惰性氣體氛圍、且0.20～0.98 MPa之壓力下進行熱處理，可於較先前更高溫下實施熱處理，從而可顯著地提高品質優異之撓性金屬貼合積層板之生產性。 本實施形態中之熱處理步驟係於惰性氣體氛圍下進行。於在大氣中進行熱處理步驟之情形時，產生在高溫下熱處理時金屬箔發生氧化之問題，於在真空中進行之情形時，積層體中所含之空氣發生膨脹，從而於表面產生鼓出。作為惰性氣體，無特別限定，例如可列舉氮氣、氬氣等，其中，就獲得性、經濟性之觀點而言，較佳為氮氣。 熱處理步驟中之壓力為0.20～0.98 MPa，較佳為0.50～0.98 MPa，更佳為0.70～0.98 MPa，進而較佳為0.90～0.98 MPa。若熱處理步驟中之壓力未達0.20 MPa，則於在高溫下進行熱處理之情形時積層板表面產生鼓出，另一方面，若壓力超過0.98 MPa，則產生設備構造變得複雜之問題。 熱處理步驟中之壓力可藉由一般之壓力計測定。 熱處理步驟中之熱處理溫度為熱塑性聚醯亞胺之Tg-20℃～Tg+50℃，較佳為Tg-20℃～Tg+30℃，更佳為Tg-10℃～Tg+30℃。若熱處理溫度未達Tg-20℃，則撓性金屬貼合積層板之生產性變差，若超過Tg+50℃，則產生鼓出或發生樹脂分解之風險變高。 熱處理步驟中之熱處理時間由於取決於熱塑性聚醯亞胺之種類、或撓性金屬貼合積層板之用途，故而無特別限定，通常為60～420分鐘，較佳為90～300分鐘，更佳為120～240分鐘。若熱處理時間為60分鐘以上，則有尺寸變化在撓性金屬積層板整體上得到均一抑制之傾向，若為420分鐘以下，則有撓性金屬積層板之生產性提高之傾向。 實施熱處理之積層體可為藉由捲取裝置捲取後之捲筒狀之積層體，亦可為解開捲筒後之平坦之片狀積層體，但就生產性之觀點而言，較佳為對捲筒狀之積層體實施熱處理。 熱處理步驟尤其較佳為於高壓釜內進行。藉由使用高壓釜，有變得容易於惰性氣體氛圍、且0.20～0.98 MPa之壓力下之條件下進行熱處理，撓性金屬貼合積層板之生產性更進一步提高之傾向。 藉由本發明之製造方法而獲得之撓性金屬積層板為尺寸變化於積層板整體上得到均一抑制者，但若考慮各材料之線膨脹係數，則該效果會變得更加顯著。具體而言，非熱塑性聚醯亞胺之線膨脹係數通常與金屬箔之線膨脹係數同等或在其以下，熱塑性聚醯亞胺之線膨脹係數變得大於金屬箔。因此，尤其是將線膨脹係數較大之熱塑性聚醯亞胺與線膨脹係數較小之非熱塑性聚醯亞胺組合而製作聚醯亞胺樹脂膜，藉此和與其貼合之金屬箔之線膨脹係數的差變小，其結果為，有尺寸變化之偏差更降低之傾向。 熱塑性聚醯亞胺之線膨脹係數較佳為20～100 ppm，更佳為30～70 ppm，進而較佳為40～60 ppm。又，非熱塑性聚醯亞胺之線膨脹係數較佳為20 ppm以下，更佳為18 ppm以下，進而較佳為16 ppm以下。 此處，線膨脹係數可藉由TMA(例如島津製作所(股)公司製造之商品名「TMA-60」)測定，於升溫速度10℃/分鐘下，基於自100℃至150℃之範圍內所獲得之測定值而求出。 於本實施形態之製造方法中，在非熱塑性聚醯亞胺層之至少單面設置含有熱塑性聚醯亞胺之接著層。此處，於僅在非熱塑性聚醯亞胺層之單面設置接著層之情形時，所獲得之撓性金屬貼合積層板成為具有非熱塑性聚醯亞胺層-接著層-金屬箔之3層構造之單面金屬貼合積層板，於在非熱塑性聚醯亞胺層之雙面設置接著層之情形時，成為具有金屬箔-接著層-非熱塑性聚醯亞胺層-接著層-金屬箔之雙面3層(5層)結構之雙面金屬貼合積層板。再者，具有接著層-非熱塑性聚醯亞胺層-接著層-金屬箔之4層構造之積層板亦包含於單面金屬貼合積層板中。 可利用金屬箔電路被覆用之覆蓋層來被覆將本實施形態中之撓性金屬貼合積層板之金屬層蝕刻為特定形狀而獲得之蝕刻面，獲得撓性印刷配線板。作為覆蓋層，只要為被覆金屬箔電路者，則並無特別限定，可使用於聚醯亞胺等膜上塗佈接著劑之覆蓋層、液狀抗蝕劑、乾膜抗蝕劑等。撓性印刷配線板例如適宜地用作IC晶片安裝用之所謂覆晶封裝撓性印刷配線板。 再者，本說明書中之各物性只要無特別詳細說明，則可根據以下實施例中所記載之方法測定。 [實施例] 以下，藉由實施例及比較例對本發明進行更具體說明，但本發明並不僅限於該等實施例。 實施例及比較例中所用之各成分、材料如下所述。 (聚醯亞胺樹脂膜) (1)聚醯亞胺樹脂膜A Kaneka公司製造之商品名「FRS－142#SW」 厚度25 μm 熱塑性聚醯亞胺之Tg＝290℃ (2)聚醯亞胺樹脂膜B Kaneka公司製造之商品名「FC-142」 厚度25 μm 熱塑性聚醯亞胺之Tg＝240℃ (銅箔) JX金屬公司製造之商品名「壓延銅箔BHY」 厚度12 μm 各評價方法及測定方法如下所述。 [玻璃轉移溫度(Tg)] 於Tg之測定中，將藉由蝕刻去除撓性銅貼合積層板之銅箔部分並使之乾燥者作為樣品。作為測定裝置，使用TA Instruments公司製造之商品名「RSA-G2」，於升溫溫度10℃/分鐘下進行測定，將所獲得之tanδ之峰值作為Tg(℃)。 [尺寸變化率] 基於JIS C 6471之9.6項進行測定。具體而言，如下測定。 自寬度500 mm之撓性金屬貼合積層板於寬度方向上切出2張樣品，如圖1所示，測定MD-L1、L2、L3、L4之長度(初始長度)。於蝕刻銅箔後，以標準狀態放置12小時以上後，再次測定MD-L1、L2、L3、L4之長度(蝕刻後長度)。根據下述式算出MD-L1、L2、L3、L4之尺寸變化率。 尺寸變化率(%)＝(蝕刻後長度－初始長度)/初始長度×100 其次，求出MD-L1、L2、L3、L4之尺寸變化率之最大值與最小值之差，將其差為0.05%以內之情形評為「○」，將超過0.05%之情形評為「×」。 [外觀(鼓出)] 以目視觀察撓性金屬貼合積層板之表面，將於熱處理前後鼓出之個數無變化之情形評為「○」，將於熱處理後鼓出之個數增加之情形評為「×」。 [判定] 將尺寸變化率、外觀之評價均為「○」者評為「○」，將任一者、或兩者之評價為「×」者評為「×」。 [實施例1] 將於雙面具有接著層之聚醯亞胺樹脂膜A、及銅箔藉由具有一對金屬輥之熱層壓裝置(YURI ROLL公司製造之商品名「撓性印刷基板用高溫貼合機」)進行貼合。將所獲得之積層體放入氮氣氛圍之高壓釜內，於溫度270℃、壓力0.9 MPa下進行120分鐘熱處理，藉此獲得具有5層構造之雙面撓性銅貼合積層板。 利用所獲得之撓性銅貼合積層板進行尺寸變化率、外觀之評價，將結果示於表1。 [實施例2～6及比較例1～5] 除改變熱處理溫度及壓力外，藉由與實施例1相同之方法獲得撓性銅貼合積層板，進行尺寸變化率、外觀之評價。將結果示於表1。 [實施例7～10、比較例6～8] 除使用聚醯亞胺樹脂膜B代替聚醯亞胺樹脂膜A，且改變熱處理溫度、壓力外，藉由與實施例1相同之方法獲得雙面撓性銅貼合積層板，而進行尺寸變化率、外觀之評價。將結果示於表2。 [表1] [表2] 自表1及表2所示之結果，可知：藉由於惰性氣體氛圍、且特定之溫度及壓力下，對將設有含有熱塑性聚醯亞胺之接著層之聚醯亞胺樹脂膜、與金屬箔貼合而獲得之積層體進行熱處理，可於短時間內效率良好地生產尺寸變化於積層板整體上得到均一抑制、且表面無鼓出之撓性金屬貼合積層板。 本案係基於在2016年6月3日向日本專利局提出申請之日本專利申請案(日本專利特願2016-111447號)者，其內容作為參照併入本文。 [產業上之可利用性] 藉由本發明之製造方法而獲得之金屬貼合積層板具有作為撓性印刷配線板所用之構件的產業上之可利用性。
圖1表示用於測定尺寸變化率之樣品之示意圖。

Claims (9)

  1. 一種撓性金屬貼合積層板之製造方法，其包括以下步驟： (a)藉由將聚醯亞胺樹脂膜與金屬箔貼合，獲得積層體，上述聚醯亞胺樹脂膜包含非熱塑性聚醯亞胺層、及含有熱塑性聚醯亞胺之接著層，且於上述非熱塑性聚醯亞胺層之至少單面設有上述接著層；及 (b)將上述步驟(a)中所獲得之積層體於惰性氣體氛圍、且0.20～0.98 Mpa之壓力下，以上述熱塑性聚醯亞胺之Tg-20℃～Tg+50℃之溫度進行熱處理。
  2. 如請求項1之製造方法，其於上述步驟(a)中，使聚醯亞胺樹脂膜與金屬箔藉由層壓而貼合。
  3. 如請求項1或2之製造方法，其中於上述步驟(b)中，以上述熱塑性聚醯亞胺之Tg-10℃～Tg+30℃之溫度進行熱處理。
  4. 如請求項1至3中任一項之製造方法，其中上述步驟(b)中之熱處理時間為60～420分鐘。
  5. 如請求項1至4中任一項之製造方法，其中於上述步驟(b)中，積層體為捲筒狀。
  6. 如請求項1至5中任一項之製造方法，其係於高壓釜內進行上述步驟(b)。
  7. 如請求項1至6中任一項之製造方法，其中上述熱塑性聚醯亞胺之Tg為240～290℃。
  8. 如請求項1至7中任一項之製造方法，其中上述撓性金屬貼合積層板為單面金屬貼合積層板。
  9. 如請求項1至7中任一項之製造方法，其中上述撓性金屬貼合積層板為雙面金屬貼合積層板。
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JP6948418B2 (ja) 2021-10-13
US10751977B2 (en) 2020-08-25
JPWO2017209060A1 (ja) 2019-02-21
JP2020104517A (ja) 2020-07-09
KR102268762B1 (ko) 2021-06-25
KR20190009796A (ko) 2019-01-29
US20190184680A1 (en) 2019-06-20
WO2017209060A1 (ja) 2017-12-07

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