JP6948418B2 - フレキシブル金属張積層板の製造方法 - Google Patents
フレキシブル金属張積層板の製造方法 Download PDFInfo
- Publication number
- JP6948418B2 JP6948418B2 JP2020011996A JP2020011996A JP6948418B2 JP 6948418 B2 JP6948418 B2 JP 6948418B2 JP 2020011996 A JP2020011996 A JP 2020011996A JP 2020011996 A JP2020011996 A JP 2020011996A JP 6948418 B2 JP6948418 B2 JP 6948418B2
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- Japan
- Prior art keywords
- thermoplastic polyimide
- laminate
- clad laminate
- metal
- manufacturing
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
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- B—PERFORMING OPERATIONS; TRANSPORTING
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- 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
- 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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- B29C65/00—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
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- B—PERFORMING OPERATIONS; TRANSPORTING
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- 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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- B—PERFORMING OPERATIONS; TRANSPORTING
- B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
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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
- B29C65/4805—Joining or sealing of preformed parts, e.g. welding of plastics materials; Apparatus therefor using adhesives, i.e. using supplementary joining material; solvent bonding characterised by the type of adhesives
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- B29C66/91941—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
- 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
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
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- H—ELECTRICITY
- H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
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- H—ELECTRICITY
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Description
また、特許文献2には、ガラス転移領域で観察される吸熱ピークの熱量を特定の範囲に調節することにより、フレキシブル金属箔積層体の熱収縮による寸法変化率およびそのバラツキを小さくできることが開示されており、そのような積層体は、樹脂のガラス転移点Tgよりも5〜50℃低い温度で8時間以上熱処理することにより得られることが記載されている。
また、特許文献2のフレキシブルプリント金属箔積層体は、8時間以上という長時間の熱処理が必要であり、生産性に劣る。また、仮に、熱処理の時間を短くするために、より高温で熱処理を行った場合、積層体中に含まれる空気が膨張することにより表面に膨れが発生し、外観に劣るという問題が生じる。
上記事情に鑑み、本発明は、積層体全体に亘って寸法変化が均一に抑制され、且つ、表面に膨れのないフレキシブル金属張積層板を効率良く生産することのできる、フレキシブル金属張積層板の製造方法を提供することを目的とする。
[1]
フレキシブル金属張積層板の製造方法であって、
(a)非熱可塑性ポリイミド層と、熱可塑性ポリイミドを含有する接着層とからなり、前記非熱可塑性ポリイミド層の少なくとも片面に前記接着層が設けられたポリイミド樹脂フィルムと、金属箔と、を貼り合わせることにより積層体を得る工程と、
(b)前記工程(a)で得られた積層体を、不活性ガス雰囲気、且つ、0.20〜0.98Mpaの圧力下、前記熱可塑性ポリイミドのTg−20℃〜Tg+50℃の温度で熱処理する工程と、
を含む、製造方法。
[2]
前記工程(a)において、ポリイミド樹脂フィルムと金属箔とをラミネートにより貼り合わせる、上記[1]記載の製造方法。
[3]
前記工程(b)において、前記熱可塑性ポリイミドのTg−10℃〜Tg+30℃の温度で熱処理する、上記[1]又は[2]記載の製造方法。
[4]
前記工程(b)における熱処理時間が60〜420分である、上記[1]〜[3]のいずれか記載の製造方法。
[5]
前記工程(b)において積層体がロール状である、上記[1]〜[4]のいずれか記載の製造方法。
[6]
前記工程(b)をオートクレーブ内で行う、上記[1]〜[5]のいずれか記載の製造方法。
[7]
前記熱可塑性ポリイミドのTgが240〜290℃である、上記[1]〜[6]のいずれか記載の製造方法。
[8]
前記フレキシブル金属張積層板が片面金属張積層板である、上記[1]〜[7]のいずれか記載の製造方法。
[9]
前記フレキシブル金属張積層板が両面金属張積層板である、上記[1]〜[7]のいずれか記載の製造方法。
フレキシブル金属張積層板の製造方法であって、
(a)非熱可塑性ポリイミド層と、熱可塑性ポリイミドを含有する接着層とからなり、前記非熱可塑性ポリイミド層の少なくとも片面に前記接着層が設けられたポリイミド樹脂フィルムと、金属箔と、を貼り合わせることにより積層体を得る工程と、
(b)前記工程(a)で得られた積層体を、不活性ガス雰囲気、且つ、0.20〜0.98Mpaの圧力下、前記熱可塑性ポリイミドのTg−20℃〜Tg+50℃の温度で熱処理する工程と、
を含む。
以下、上記工程(a)及び工程(b)を、それぞれ「積層工程」及び「熱処理工程」ともいう。
本実施形態の製造方法における工程(a)は、非熱可塑性ポリイミド層と、熱可塑性ポリイミドを含有する接着層とからなり、前記非熱可塑性ポリイミド層の少なくとも片面に前記接着層が設けられたポリイミド樹脂フィルムと、金属箔と、を貼り合わせることにより積層体を得る工程である。
なお、本明細書において、ガラス転移温度(Tg)は、動的粘弾性測定装置(DMA)により測定した貯蔵弾性率の変曲点の値により求めることができ、具体的には、後述する実施例の方法に従って測定することができる。
上記(i)の方法の場合、ポリイミド樹脂フィルムは、例えば、非熱可塑性ポリイミド層の少なくとも片面に、熱可塑性ポリイミドの前駆体であるポリアミック酸溶液を塗布し、加熱、乾燥してイミド化することにより得ることができる。
本実施形態における工程(b)は、前記工程(a)で得られた積層体を、不活性ガス雰囲気、且つ、0.20〜0.98MPaの圧力下で、前記熱可塑性ポリイミドのTg−20℃〜Tg+50℃の温度で熱処理する工程である。
本発明者らは、金属箔と基材樹脂との間に熱可塑性ポリイミドを含む接着層を設け、得られた積層体を不活性ガス雰囲気、且つ、0.20〜0.98MPaの圧力下で熱処理することで、従来よりも高温で熱処理を実施することが可能となり、品質に優れたフレキシブル金属張積層板の生産性を著しく向上させることができることを見出した。
熱処理工程における圧力は、一般的な圧力計により測定することができる。
ここで、線膨張係数は、TMA(例えば、(株)島津製作所社製 商品名「TMA−60」)により測定することができ、昇温速度10℃/分で、100℃から150℃の範囲に得られた測定値より求める。
(ポリイミド樹脂フィルム)
(1)ポリイミド樹脂フィルムA
カネカ社製 商品名「FRS−142#SW」 厚さ25μm
熱可塑性ポリイミドのTg=290℃
(2)ポリイミド樹脂フィルムB
カネカ社製 商品名「FC−142」 厚さ25μm
熱可塑性ポリイミドのTg=240℃
(銅箔)
JX金属社製 商品名「圧延銅箔BHY」 厚さ12μm
Tgの測定においては、フレキシブル銅張積層板の銅箔部分をエッチングにより除去し、乾燥させたものをサンプルとした。測定装置としてはTA Instruments社製 商品名「RSA−G2」を用い、昇温温度10℃/分で測定を行い、得られたtanδのピークをTg(℃)とした。
JIS C 6471の9.6項に準拠して測定した。具体的には以下のとおりに測定した。
フレキシブル金属張積層板500mm幅から幅方向に2枚サンプルを切り出し、図1に示すとおり、MD−L1、L2、L3、L4の長さを測定した(初期長さ)。銅箔エッチング後、標準状態で12時間以上放置した後、再びMD−L1、L2、L3、L4の長さを測定した(エッチング後長さ)。MD−L1、L2、L3、L4の寸法変化率を下記式に従って算出した。
寸法変化率(%)=(エッチング後長さ−初期長さ)/初期長さ×100
次いで、MD−L1、L2、L3、L4の寸法変化率の最大値と最小値の差を求め、その差が0.05%以内である場合を「○」と評価し、0.05%を超える場合を「×」と評価した。
フレキシブル金属張積層板の表面を目視により観察し、熱処理前後で膨れの個数に変化がなかった場合を「○」と評価し、熱処理後に膨れの個数が増えた場合を「×」と評価した。
寸法変化率、外観の評価が共に「○」であったものを「○」と評価し、どちらか一方、或いは両方の評価が「×」であったものを「×」と評価した。
両面に接着層を有するポリイミド樹脂フィルムAと、銅箔とを、一対の金属ロールを有する熱ラミネート装置(由利ロール社製 商品名「フレキシブルプリント基板用高温ラミネーター」)により貼り合わせた。得られた積層体を、窒素ガス雰囲気のオートクレーブ内に入れ、温度270℃、圧力0.9MPaで120分熱処理を行うことにより、5層構造を有する両面フレキシブル銅張積層板を得た。
得られたフレキシブル銅張積層板を用いて寸法変化率、外観の評価を行い、結果を表1に示した。
熱処理温度および圧力を変えたこと以外は実施例1と同様の方法によりフレキシブル銅張積層板を得て、寸法変化率、外観の評価を行った。結果を表1に示す。
ポリイミド樹脂フィルムAの代わりにポリイミド樹脂フィルムBを用い、熱処理温度、圧力を代えたこと以外は実施例1と同様の方法により両面フレキシブル銅張積層板を得て、寸法変化率、外観の評価を行った。結果を表2に示す。
Claims (9)
- フレキシブル金属張積層板の製造方法であって、
(a)線膨張係数が20ppm以下の非熱可塑性ポリイミド層と、線膨張係数が20〜100ppmの熱可塑性ポリイミドを含有する接着層とからなり、前記非熱可塑性ポリイミド層の少なくとも片面に前記接着層が設けられたポリイミド樹脂フィルムと、金属箔と、を貼り合わせることにより積層体を得る工程と、
(b)前記工程(a)で得られた積層体を、不活性ガス雰囲気、且つ、0.20〜0.90MPaの圧力下、前記熱可塑性ポリイミドのTg−20℃〜Tg+50℃の温度で熱処理する工程と、
を含む、製造方法。 - 前記工程(a)において、ポリイミド樹脂フィルムと金属箔とをラミネートにより貼り合わせる、請求項1記載の製造方法。
- 前記工程(b)において、前記熱可塑性ポリイミドのTg−10℃〜Tg+30℃の温度で熱処理する、請求項1又は2記載の製造方法。
- 前記工程(b)における熱処理時間が60〜420分である、請求項1〜3のいずれか1項記載の製造方法。
- 前記工程(b)において積層体がロール状である、請求項1〜4のいずれか1項記載の製造方法。
- 前記工程(b)をオートクレーブ内で行う、請求項1〜5のいずれか1項記載の製造方法。
- 前記熱可塑性ポリイミドのTgが240〜290℃である、請求項1〜6のいずれか1項記載の製造方法。
- 前記フレキシブル金属張積層板が片面金属張積層板である、請求項1〜7のいずれか1項記載の製造方法。
- 前記フレキシブル金属張積層板が両面金属張積層板である、請求項1〜7のいずれか1項記載の製造方法。
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JP4731107B2 (ja) | 2003-10-17 | 2011-07-20 | 日本メクトロン株式会社 | フレキシブル金属箔積層体 |
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JP4410021B2 (ja) * | 2004-04-19 | 2010-02-03 | 株式会社カネカ | 生産性が向上されたフレキシブル金属張積層板の製造方法ならびにそれにより得られるフレキシブル金属張積層板 |
KR100952796B1 (ko) * | 2004-09-24 | 2010-04-14 | 가부시키가이샤 가네카 | 신규한 폴리이미드 필름 및 이를 이용하여 얻어지는 접착필름, 플렉시블 금속장 적층판 |
JP5069847B2 (ja) * | 2005-04-27 | 2012-11-07 | 株式会社カネカ | 新規なポリイミドフィルム並びにそれを用いて得られる接着フィルム、フレキシブル金属張積層板 |
JP4692758B2 (ja) * | 2006-02-24 | 2011-06-01 | 信越化学工業株式会社 | フレキシブル積層板及びその製造方法 |
JP5162379B2 (ja) * | 2008-08-29 | 2013-03-13 | 株式会社有沢製作所 | ポリアミック酸及び非熱可塑性ポリイミド樹脂 |
KR20100048474A (ko) * | 2008-10-31 | 2010-05-11 | 에스케이에너지 주식회사 | 연성금속박적층체 및 이의 제조방법 |
JP5524475B2 (ja) | 2008-11-28 | 2014-06-18 | 株式会社有沢製作所 | 2層両面フレキシブル金属積層板及びその製造方法 |
JP5364414B2 (ja) * | 2009-03-30 | 2013-12-11 | 三井化学株式会社 | ポリイミド樹脂組成物、それを用いた金属積層体 |
KR101416782B1 (ko) * | 2012-04-24 | 2014-07-08 | 에스케이이노베이션 주식회사 | 연성 금속박 적층체 |
JP6297011B2 (ja) * | 2014-08-28 | 2018-03-20 | 株式会社有沢製作所 | 3層フレキシブル金属張積層板及び両面3層フレキシブル金属張積層板 |
JP5918822B2 (ja) | 2014-09-18 | 2016-05-18 | 株式会社カネカ | 寸法安定性を向上させたフレキシブル金属張積層板の製造方法ならびにそれにより得られるフレキシブル金属張積層板 |
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CN109219513B (zh) | 2021-03-09 |
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JP6917987B2 (ja) | 2021-08-11 |
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US20190184680A1 (en) | 2019-06-20 |
JPWO2017209060A1 (ja) | 2019-02-21 |
TWI784955B (zh) | 2022-12-01 |
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