WO2010098324A1 - 半導体装置の製造方法 - Google Patents

半導体装置の製造方法 Download PDF

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Publication number
WO2010098324A1
WO2010098324A1 PCT/JP2010/052772 JP2010052772W WO2010098324A1 WO 2010098324 A1 WO2010098324 A1 WO 2010098324A1 JP 2010052772 W JP2010052772 W JP 2010052772W WO 2010098324 A1 WO2010098324 A1 WO 2010098324A1
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WIPO (PCT)
Prior art keywords
semiconductor chip
bumps
adhesive film
insulating resin
bump
Prior art date
Application number
PCT/JP2010/052772
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English (en)
French (fr)
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WO2010098324A9 (ja
Inventor
和典 濱崎
孝 ▲松▼村
佐藤　大祐
須賀　保博
Original Assignee
ソニーケミカル＆インフォメーションデバイス株式会社
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Application filed by ソニーケミカル＆インフォメーションデバイス株式会社 filed Critical ソニーケミカル＆インフォメーションデバイス株式会社
Priority to KR1020117019916A priority Critical patent/KR101232409B1/ko
Priority to CN201080009458.3A priority patent/CN102334182B/zh
Priority to EP10746205.3A priority patent/EP2402985A4/en
Priority to US13/131,427 priority patent/US9368374B2/en
Publication of WO2010098324A1 publication Critical patent/WO2010098324A1/ja
Publication of WO2010098324A9 publication Critical patent/WO2010098324A9/ja
Priority to US15/155,228 priority patent/US9524949B2/en

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Abstract

　半導体チップと基板に絶縁性樹脂接着フィルム（ＮＣＦ）を使用してフリップチップ実装する半導体装置の製造方法において、熱プレスの際に、ＮＣＦのはみ出しと、バンプと電極パッドとの間に絶縁性樹脂や無機フィラーが介在することを防ぎ、得られる半導体装置が十分な耐吸湿リフロー性を示す製造方法を提供する。具体的には、半導体チップのペリフェラル配置された複数のバンプで囲まれた領域の面積の６０～１００％に相当する大きさと、２×１０２～１×１０５Ｐａ・ｓの最低溶融粘度とを有するＮＣＦを、バンプに対応した基板の複数の電極で囲まれた領域に仮貼りする。次に、該バンプとそれに対応する電極とが対向するように、半導体チップと基板とを位置合わせし、半導体チップ側から熱プレスする。これにより、バンプと電極とを金属結合させ、ＮＣＦを溶融させ、更に熱硬化させる。これにより半導体装置を得る。

Description

半導体装置の製造方法
　本発明は、ペリフェラル配置の複数のバンプを有する半導体チップを、絶縁性樹脂接着フィルムを介して基板にフリップチップ実装して半導体装置を取得する半導体装置の製造方法に関する。
　半導体チップを、導電粒子を含有する異方性導電接着フィルム（ＡＣＦ）を用いて基板にフリップチップ実装して半導体装置を製造することが広く行われているが、配線ピッチのファイン化が進み、導電粒子の粒径と配線ピッチとの関係で、接続信頼性を確保することが困難になってきている。
　このため、微細に作成可能な金スタッドバンプを半導体チップに設け、その半導体チップを、絶縁性樹脂接着フィルムを介して基板にフリップチップ実装することが行われるようになっている（特許文献１）。このような絶縁性樹脂接着フィルムを介してフリップチップ実装する場合、一般に、半導体チップと略同一の面積からわずかに大きな面積の絶縁性樹脂接着フィルムを基板に仮貼りした後、半導体チップと配線基板とを位置合わせし、半導体チップ側から熱プレスすることにより実装している。
特開２００８－２０３４８４号公報
　しかしながら、特許文献１のようにフリップチップ実装した場合、図５に示すように、バンプ１００を備えた半導体チップ１０１の外縁から、溶融した絶縁性樹脂接着フィルム（ＮＣＦ）１０２がはみ出し、はみ出した樹脂が熱プレスボンダー１０３に付着し、熱プレスの際に圧力過大となり、意図した品質の半導体装置が得られない場合があるという問題があった。また、熱プレス後に、基板１０４の電極１０５と半導体チップ１０１のバンプ１００との間から、絶縁性樹脂や無機フィラーを排除しきれないために、それらの間に満足の行く金属結合が形成できず、接続信頼性が大きく低下する場合があるという問題もあった。更に、吸湿リフロー後に、絶縁性樹脂接着フィルム１０２が外界に露出しているために、硬化不良や半導体チップ１０１の浮きの問題が生じ、この点からも接続信頼性が低下する場合があるという問題もあった。
　本発明は、以上の従来の技術の課題を解決しようとするものであり、半導体チップと基板に絶縁性樹脂接着フィルムを使用してフリップチップ実装する半導体装置の製造方法において、熱プレスの際に、溶融した絶縁性樹脂接着フィルムのはみ出しと、バンプと電極パッドとの間に絶縁性樹脂や無機フィラーが介在することを防ぎ、得られる半導体装置が十分な耐吸湿リフロー性を示す製造方法を提供することを目的とする。
　本発明者は、半導体チップのペリフェラル配置された複数のバンプで囲まれた領域の面積に対する絶縁性樹脂接着フィルムの面積と絶縁性樹脂接着フィルムの最低溶融粘度とをそれぞれ特定範囲に設定することにより、上述の目的を達成できることを見出し、本発明を完成させるに至った。
　即ち、本発明は、ペリフェラル配置の複数のバンプを有する半導体チップを、該バンプに対応した複数の電極を有する基板に、絶縁性樹脂接着フィルムを介してフリップチップ実装することにより半導体装置を製造する方法において、
　半導体チップのペリフェラル配置された複数のバンプで囲まれた領域の面積の６０～１００％に相当する大きさと、２×１０２～１×１０５Ｐａ・ｓの最低溶融粘度とを有する絶縁性樹脂接着フィルムを、該バンプに対応した基板の複数の電極で囲まれた領域に仮貼りし、該バンプとそれに対応する電極とが対向するように、半導体チップと基板とを位置合わせし、半導体チップ側から熱プレスすることにより、バンプと電極とを金属結合させ、絶縁性樹脂接着フィルムを溶融させ、更に熱硬化させることを特徴とする製造方法を提供する。
　本発明の半導体装置の製造方法においては、半導体チップのペリフェラル配置された複数のバンプで囲まれた領域の面積の少なくとも６０～１００％に相当する大きさと、２×１０２～１×１０５Ｐａ・ｓの最低溶融粘度とを有する絶縁性樹脂接着フィルムを、半導体チップの複数のバンプに対応する基板の複数の電極に囲まれた領域に仮貼りする。従って、半導体チップを基板に熱プレスした直後は、半導体チップのバンプとそれに対応した基板の電極パッドとの間には絶縁性樹脂接着フィルムが存在せず、また、半導体チップの外側に溶融した絶縁性樹脂接着フィルムがはみ出さないようにすることができる。更に、熱プレスの際、比較的低い圧力で行うことが可能となる。従って、すべてのバンプを対応する接続パッドに十分に金属結合させることができ、熱プレスボンダーへの溶融した樹脂の付着も防止できる。また、前述したように、熱プレス後に、樹脂のはみ出しを生じさせることなく、半導体チップのバンプと基板の電極との接合部を封止でき、耐吸湿リフロー性を向上させることが可能となる。よって、高い接続信頼性の半導体装置を得ることができる。
バンプを備えた半導体チップの断面図である。 半導体チップのバンプ側平面図である。 電極を備えた基板の断面図である。 絶縁性樹脂接着フィルムを仮貼りした基板の断面図である。 絶縁性樹脂接着フィルムを仮貼りした基板の絶縁性樹脂接着フィルム側平面図である。 基板に半導体チップを熱プレスボンダーで熱プレス直後の説明図である。 基板に半導体チップを熱プレスボンダーで十分に熱プレスした後の説明図である。 従来技術のフリップチップ実装の説明図である。
　本発明の半導体装置の製造方法を図面を参照しながら説明する。
（１）　まず、バンプ１を備えた半導体チップ２（図１Ａ）と、電極１１を備えた基板１２（図２）と、絶縁性樹脂接着フィルム（ＮＣＦ）とを用意する。
　半導体チップ２において、バンプ１は半導体チップ２の外周縁近くにペリフェラル配置、即ち、一列のバンプ列として配置されている（図１Ｂ）。図１Ｂでは、一列のバンプ列であるが、二列以上のバンプ列であってもよい。
　半導体チップ２やバンプ１としては特に制限はないが、バンプ１については、ファインピッチ化に高度に対応できる点から、金スタッドバンプを好ましく利用することができる。このような金スタッドバンプの大きさに関し、その高さは、好ましくは３５～１００μｍ、より好ましくは３５～７０μｍ、特に好ましくは３５～４５μｍである。また、その底径は、好ましくは１０～５０μｍ、より好ましくは１０～４０μｍ、特に好ましくは１０～２０μｍである。また、バンプ間ピッチは、好ましくは５０～２００μｍ、より好ましくは５０～７０μｍである。
　半導体チップ２の外周縁とバンプ１との距離は、溶融した絶縁性樹脂のはみ出しを防ぐために、好ましくは０．０７～０．２ｍｍ、より好ましくは０．１～０．１５ｍｍに設定する。
　基板１２において、電極１１は、接続すべき半導体チップ２のバンプ１（バンプ列）に対応するように配置される。そして、この複数の電極に囲まれた領域に絶縁性樹脂接着フィルム（ＮＣＦ）が仮貼りされる。
　基板１２や電極１１としては、特に限定されず、例えば基板１２としては、リジッド基板、フレキシブル基板、リジッドフレキシブル基板などを使用することができる。電極１１としては、例えば、銅箔をランド状に成形し、表面にＮｉ／Ａｕメッキしたものを使用することができる。
　絶縁性樹脂接着フィルム（ＮＣＦ）としては、半導体チップを基板に実装する際に使用される公知の絶縁性樹脂接着フィルムを使用することができ、例えば、エポキシ系硬化型樹脂組成物やアクリル系硬化型樹脂組成物をフィルム状に成形したものが挙げられる。これらは、熱硬化型のものを好ましく使用することができる。
　エポキシ系熱硬化型樹脂組成物は、例えば、分子内に２つ以上のエポキシ基を有する化合物もしくは樹脂、エポキシ硬化剤、成膜成分等から構成される。
　分子内に２つ以上のエポキシ基を有する化合物もしくは樹脂としては、液状であっても、固体状であってもよく、ビスフェノールＡ型エポキシ樹脂やビスフェノールＦ型エポキシ樹脂などの二官能エポキシ樹脂、フェノールノボラック型エポキシ樹脂やクレゾールノボラック型エポキシ樹脂などのノボラック型エポキシ樹脂などを例示できる。また、３，４－エポキシシクロヘキセニルメチル－３´，４´－エポキシシクロヘキセンカルボキシレート等の脂環式エポキシ化合物も使用することができる。
　エポキシ硬化剤としては、例えば、アミン系硬化剤、イミダゾール系硬化剤、酸無水物系硬化剤、スルホニウムカチオン系硬化剤等が挙げられる。硬化剤は潜在性であってもよい。
　成膜成分としては、例えば、エポキシ化合物やエポキシ樹脂と相溶するフェノキシ樹脂やアクリル樹脂を挙げることができる。
　エポキシ系熱硬化型樹脂組成物は、必要に応じて公知の硬化促進剤、シランカップリング剤、金属捕捉剤、ブタジエンゴム等の応力緩和剤、シリカなどの無機フィラー、ポリイソシアネート系架橋剤、着色料、防腐剤、溶剤等を含有することができる。
　アクリル系熱硬化型樹脂組成物は、例えば、（メタ）アクリレートモノマー、成膜用樹脂、シリカなどの無機フィラー、シランカップリング剤、ラジカル重合開始剤等から構成される。
　（メタ）アクリレートモノマーとしては、単官能（メタ）アクリレートモノマー、多官能（メタ）アクリレートモノマー、あるいはそれらにエポキシ基、ウレタン基、アミノ基、エチレンオキサイド基、プロピレンオキサイド基等を導入した変性単官能または多官能（メタ）アクリレートモノマーを使用することができる。また、本発明の効果を損なわない限り、（メタ）アクリレートモノマーとラジカル共重合可能な他のモノマー、例えば（メタ）アクリル酸、酢酸ビニル、スチレン、塩化ビニル等を併用することができる。
　アクリル系熱硬化型樹脂組成物用の成膜用樹脂としては、フェノキシ樹脂、ポリビニルアセタール樹脂、ポリビニルブチラール樹脂、アルキル化セルロース樹脂、ポリエステル樹脂、アクリル樹脂、スチレン樹脂、ウレタン樹脂、ポリエチレンテレフタレート樹脂等が挙げられる。
　ラジカル重合開始剤としては、ベンゾイルパーオキサイド、ジクミルパーオキサイド、ジブチルパーオキサイド等の有機過酸化物、アゾビスイソブチロニトリル、アゾビスバレロニトリル等のアゾビス系化合物を挙げることができる。
　アクリル系熱硬化型樹脂組成物は、必要に応じ、ブタジエンゴム等の応力緩和剤や、酢酸エチル等の溶剤、着色料、酸化防止剤、老化防止剤等を含有することができる。
　これらのエポキシ系熱硬化型樹脂組成物やアクリル系熱硬化型樹脂組成物から絶縁性樹脂接着フィルム（ＮＣＦ）への成形は、公知の手法を使用して行うことができる。
　以上説明した本発明で使用する絶縁性樹脂接着フィルム（ＮＣＦ）については、その最低溶融粘度を２×１０２～１×１０５Ｐａ・ｓ、好ましくは５×１０２～５×１０４Ｐａ・ｓに設定する必要がある。この範囲よりも低粘度となると、はみ出しが生ずる可能性が増加し、高粘度となるとバンプと電極との接合部を封止できなくなる可能性が増加するからである。
　また、絶縁性樹脂接着フィルム（ＮＣＦ）の厚みは、薄すぎると取り扱い性が低下し、アンダーフィルの機能も果たせなくなり、厚すぎると熱プレスの際のはみ出しが生ずるので、好ましくは３０～７０μｍ、より好ましくは３５～５０μｍである。
（２）　次に、基板１２に、２×１０２～１×１０５Ｐａ・ｓの最低溶融粘度を有する絶縁性樹脂接着フィルム（ＮＣＦ）を仮貼りする（図３Ａ）。この仮貼りの位置は、半導体チップ２のペリフェラル配置の複数のバンプ１で囲われた領域Ｒの内側に対応する位置である（図３Ｂ）。
　ここで、絶縁性樹脂接着フィルム（ＮＣＦ）の大きさは、半導体チップ２のペリフェラル配置されたバンプ１で囲まれた領域Ｒの面積の６０～１００％、好ましくは７０～９０％に相当する大きさである。６０％未満となると、半導体チップのバンプと基板の電極との接合部を封止できなくなる可能性が増大し、１００％を超えるとバンプと電極との間に排除しきれない絶縁性樹脂や無機フィラーが残存するおそれがあり、しかも、熱プレス条件を低下させることができない。
　仮貼りの条件としては、絶縁性樹脂接着フィルムが実質的に硬化しないような条件で行うことが好ましく、具体的には、温度６０～７０℃、圧力０．２５～１．０ＭＰａ、１～３秒という条件を挙げることができる。
（３）　次に、バンプ１とそれに対応する電極１１とが対向するように、半導体チップ２と基板１２とを位置合わせし、半導体チップ２側から、熱プレスボンダー３０で熱プレスする（図４Ａ）。この場合、まず、バンプ１と電極１１とが、絶縁性樹脂接着フィルムを介さずに直接接触するので、両者の間に金属結合を形成させる。絶縁性樹脂接着フィルムについては、溶融させ、更に熱硬化させる。これにより、半導体装置を得ることができる。この熱プレスの際、溶融した絶縁性樹脂接着フィルムは、半導体チップ２の外縁に向かって拡がり、更に硬化する。硬化した絶縁性樹脂接着フィルムの周縁は、ペリフェラル配置の複数のバンプ１で囲まれた領域内のみに存在してもよいが、図４Ｂに示すように、ペリフェラル配置の複数のバンプ１と半導体チップ２の外縁との間に存在することが、バンプ１と電極１１との接合部を封止できる点で好ましい。
　熱プレスボンダー３０としては、従来よりフリップチップ実装の際に使用されている熱プレスボンダーを使用することができる。
　このような熱プレスボンダー３０を使用する本発明における熱プレス条件は、熱プレスの温度が好ましくは１２０～２７０℃、より好ましくは１７０～２００℃である。圧力が好ましくは０．５～２．５ＭＰａ、より好ましくは２．０～２．５ＭＰａである。特に、本発明の構成により、熱プレス時の圧力を、従来が１０ｋｇ／ＩＣであるところ、約１／３～１／５の圧力に低減させることができる。
　以上説明した本発明の製造方法により得られる半導体装置は、吸湿リフロー耐性を有する、優れた接続信頼性を示すものとなる。
　以下、本発明を実施例により具体的に説明する。なお、以下の実施例において、ＮＣＦ用組成物の最低溶融粘度は、コーン／プレート粘度計を用いて測定した。
絶縁性樹脂接着フィルム（ＮＣＦ）の製造例１～５
　表１の成分を均一に混合し、その混合物に、固形分濃度が６０質量％となるようにトルエンを添加して混合してＮＣＦ用組成物を得た。得られた組成物を、バーコータを用いて剥離フィルム（ソニーケミカル＆インフォメーションデバイス株式会社製）に塗布し、８０℃のオーブン中で乾燥し、５０μｍ厚の絶縁性樹脂接着フィルム（ＮＣＦ）１～５を得た。得られたＮＣＦの最低溶融粘度（Ｐａ・ｓ）はコーン／プレート粘度計を使用して、昇温速度１０℃／ｍｉｎにて測定し、得られた結果を表１に示す。なお、最低溶融粘度の観点から、本発明に適用可能な絶縁性樹脂接着フィルムはＮＣＦ２～４である。
　
　
　
　
Figure JPOXMLDOC01-appb-T000001
 表注
*1　フェノキシ樹脂、東都化成社製
*2　東都化成社製
*3　ジャパンエポキシレジン社製
*4　アクリロニトリルブタジエンゴム粒子、日本合成ゴム社製
*5　イミダゾール系潜在性硬化剤、旭化成ケミカルズ社製
*6　信越石英社製
*7　日本アエロジル社製
*8　モメンティブ・パーフォーマンス・マテリアルズ社製
　　実施例１～７及び比較例１～６
　ペリフェラル配置の複数のＡｕスタッドバンプ（７５～８５μｍ高；１５０μｍピッチ）が設けられたられたＬＳＩチップ（６．３ｍｍ角、０．１ｍｍ厚；バンプとＬＳＩチップ周縁との平均距離０．１μｍ）の当該バンプに対応した電極（銅にニッケル／金メッキしたもの）を有する基板（MCL-E-679F、日立化成工業社）の電極に囲まれた領域に、表２に示すＮＣＦ面積率にカットしたＮＣＦ１～５を、熱プレスボンダー（ソニーケミカル＆インフォメーションデバイス社）で仮貼りした（温度６０℃、圧力０．５ＭＰａ、加熱加圧時間３秒）。ここで、ＮＣＦ面積率とは、複数のバンプで囲まれた領域の面積に対する切り出したＮＣＦの面積の割合である。
（ボンダーへの樹脂付着の有無）
　ＮＣＦを仮貼りした基板の電極面に対し、ＬＳＩチップのバンプ面を対向させ、位置合わせした後に、８ｍｍ角の熱プレスボンダー（ソニーケミカル＆インフォメーションデバイス社）で熱プレス（本熱圧着：温度１８０℃、圧力２．５ＭＰａ、加熱加圧時間２０秒）し、半導体装置を得た。得られた半導体装置について、熱プレスボンダーへの樹脂の付着の有無を目視にて観察した。得られた結果を表２に示す。
（吸湿・リフロー耐性）
　半導体装置を、温度８５℃、湿度８５％の条件下に１６８時間放置し、最高２６５℃のハンダリフロー炉に浸漬した後の導通抵抗値を測定し、０．１３Ω未満をＡ、０．１３Ω以上１．０Ω未満をＢ、１．０Ω以上をＣと評価した。得られた結果を表２に示す。
（初期導通抵抗及びＰＣＴ後の導通抵抗）
　また、初期導通抵抗とＰＣＴ試験（１２１℃、湿度１００％の環境下に１２０時間放置）後の導通抵抗を測定した。得られた結果（複数の測定結果のうちの最大の数値）を表２に示す。なお、１Ω以上の導通抵抗の場合をオープン（ｏｐｅｎ）とした。実用上、導通抵抗は０．３Ω以下であることが望まれる。
　
　
　
　
　
　
　
　
　
　
　
Figure JPOXMLDOC01-appb-T000002
  
 
　表２からわかるように、ＮＣＦ面積率が６０～１００％に相当する大きさと、２×１０２～１×１０５Ｐａ・ｓの最低溶融粘度とを有するＮＣＦを使用した実施例１～７の半導体基板は、熱プレス時に絶縁性樹脂のはみ出しがなく、初期およびＰＣＴ試験後のそれぞれの時点での導電抵抗が低く、高い接続信頼性を実現していることがわかった。特に、実施例１～３の場合、ＰＣＴ試験後の導通抵抗が初期導通抵抗と大差なく、吸湿・リフロー耐性に優れていることがわかった。
　それに対し、比較例１、５の場合、ＮＣＦの最低溶融粘度が低すぎるため、比較例４の場合、ＮＣＦの面積率が高すぎるため、ボンダーへの樹脂の付着が観察され、吸湿・リフロー耐性も「Ｃ」評価であり、ＰＣＴ後の導通抵抗も「ｏｐｅｎ」であった。比較例４の場合、それらに加え、初期導通抵抗も「ｏｐｅｎ」であった。比較例２、６の場合、ＮＣＦの最低溶融粘度が高すぎるため、吸湿・リフロー耐性が「Ｃ」評価であり、ＰＣＴ後の導通抵抗が「ｏｐｅｎ」であった。比較例３の場合、ＮＣＦの面積率が低すぎるため、吸湿・リフロー耐性が「Ｃ」評価であり、初期並びにＰＣＴ後の導通抵抗が共に「ｏｐｅｎ」であった。
（低圧圧着性評価）
　熱プレス時の圧力を０．５ＭＰａに設定すること以外は、実施例１及び２の条件での測定をそれぞれ繰り返したところ、ボンダーへの樹脂の付着は観察されず、しかも、ＰＣＴ試験後の導通抵抗も変化しなかった。従って、本発明の製造方法は、低圧圧着に適していることがわかった。
　本発明の半導体装置の製造方法によれば、熱プレスの際に、ＮＣＦのはみ出しと、バンプと電極パッドとの間に絶縁性樹脂や無機フィラーが介在することを防ぎ、十分な耐吸湿リフロー性を示す半導体装置を提供することができる。
１、１００　バンプ
２、１０１　半導体チップ
１１、１０５　電極
１２、１０４　基板
３０、１０３　熱プレスボンダー
ＮＣＦ、１０２　絶縁性樹脂接着フィルム
Ｒ　領域

Claims (7)

  1. 　ペリフェラル配置の複数のバンプを有する半導体チップを、該バンプに対応した複数の電極を有する基板に、絶縁性樹脂接着フィルムを介してフリップチップ実装することにより半導体装置を製造する方法において、
    　半導体チップのペリフェラル配置された複数のバンプで囲まれた領域の面積の６０～１００％に相当する大きさと、２×１０２～１×１０５Ｐａ・ｓの最低溶融粘度とを有する絶縁性樹脂接着フィルムを、該バンプに対応した基板の複数の電極で囲まれた領域に仮貼りし、該バンプとそれに対応する電極とが対向するように、半導体チップと基板とを位置合わせし、半導体チップ側から熱プレスすることにより、バンプと電極とを金属結合させ、絶縁性樹脂接着フィルムを溶融させ、更に熱硬化させることを特徴とする製造方法。
  2. 　半導体チップのペリフェラル配置されたバンプ列で囲まれた領域の面積の７０～９０％を被覆するように、絶縁性樹脂接着フィルムを基板に仮貼りする請求項１記載の製造方法。
  3. 　半導体チップのバンプが、高さ３５～１００μｍの金スタッドバンプである請求項１または２記載の製造方法。
  4. 　絶縁性樹脂接着フィルムが、エポキシ系硬化型樹脂組成物またはアクリル系硬化型樹脂組成物を含有する請求項１～３のいずれかに記載の製造方法。
  5. 　絶縁性樹脂接着フィルムの厚みが、３０～７０μｍである請求項１～４のいずれかに記載の製造方法。
  6. 　熱プレスの際に、溶融した絶縁性樹脂接着フィルムが、半導体チップの外縁に向かって拡がり、硬化した後にその周縁が、ペリフェラル配置の複数のバンプと半導体チップの外縁との間に存在する請求項１～５のいずれかに記載の製造方法。
  7. 　熱プレスの温度が１２０～２７０℃であり、圧力が０．５～２．５ＭＰａである請求項１～６のいずれかに記載の製造方法。
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