JP3571767B2 - Method for producing tow prepreg and sheet prepreg - Google Patents

Method for producing tow prepreg and sheet prepreg Download PDF

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Publication number
JP3571767B2
JP3571767B2 JP21142694A JP21142694A JP3571767B2 JP 3571767 B2 JP3571767 B2 JP 3571767B2 JP 21142694 A JP21142694 A JP 21142694A JP 21142694 A JP21142694 A JP 21142694A JP 3571767 B2 JP3571767 B2 JP 3571767B2
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Japan
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tow
resin
producing
width
prepreg according
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JP21142694A
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JPH0873630A (en
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高志 瀧川
家嗣 山藤
禎仁 中原
稔之 伊藤
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Mitsubishi Chemical Corp
Mitsubishi Rayon Co Ltd
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Mitsubishi Chemical Corp
Mitsubishi Rayon Co Ltd
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Description

【0001】
【産業上の利用分野】
本発明は、繊維強化複合材料に用いられるトウプリプレグ及び複数本のトウからなるシート状プリプレグ(テープ状プリプレグを含む)の製造方法に関する。
【0002】
【従来の技術】
繊維強化複合材料に用いられる中間材料は一般的にプリプレグとよばれ、離型紙の上に樹脂を薄くコートしたホットメルトフィルムの上に強化繊維トウを引き揃え、その上からトップフィルムをかぶせるか、あるいはさらにホットメルトフィルムを上から重ねた後、加熱及び/又は加圧して強化繊維トウの構成フィラメントに樹脂を含浸させ、しかる後巻取って製造するのが一般的な製法である。
代表的な例として、上下からホットメルトフィルムで挟み込んで樹脂を含浸させる方法が特開平3−149230号公報及び特公平4−5057号公報に開示されている。
【0003】
上記公報に開示された方法は、多数本の強化繊維トウを取扱い、広幅で離型紙等の保護フィルムにはさんであるので製造プロセス上の汚れもなく安定的に製造できるメリットがある。
また一本のトウにホットメルトの樹脂を含浸させるトウプリプレグの製造方法が特公平5−80330公報に開示されており、この方法は離型紙やホットメルトフィルムを取り去ってトウ単位でプリプレグを製造する方法である。
【0004】
【発明が解決しようとする課題】
しかしながら、上記特開平3−149230号公報及び特公平4−5057号公報に開示された方法で製造されるプリプレグは、幅方向に広幅でみると樹脂含有量の変動は非常に少ないが、トウ1本程度の細幅でみると樹脂含有量の変動が大きく、広幅で製造したプリプレグを細幅で裁断して使用すると、プリプレグ間の樹脂含有量の変動が大きくなりすぎるという問題が生じる。これは多数本のトウ幅の厳密な制御はできていないので、ホットメルトフィルムの単位面積当たりの樹脂量が一定でも、トウの広がりの変動からくる単位体積当たりの繊維量の変動があるため、樹脂含浸後の単位面積当たりの樹脂含有量(重量%)が変動し、プリプレグを広幅で使用すると樹脂含有量は変動が相殺されて精度が良くなるが、例えば広幅のプリプレグをトウ1〜5本程度の広がりに相当する幅で裁断したスリットテープや、広幅のプリプレグからトウ1〜5本程度を引き剥してトウプリプレグとした場合樹脂含有量の変動が大きくなるからである。
【0005】
更に樹脂含浸速度に関して言えば、トウを横並びに置き、しかも上下から離型紙等の保護シートで押さえつけているため、トウを構成するフィラメントの移動はほとんど不可能で、樹脂の含浸速度は離型紙を介した上下からの加熱、加圧条件及び熱硬化性樹脂であれば樹脂のライフとの兼ね合いで決定され、単に加熱低粘度化すればよいというわけではなく、含浸させる工程の長さ等の問題もあり、生産速度の向上には限界があった。さらに上下からホットメルトフィルムで挟み込んだ場合はトウ内に空気が取り残されるため含浸不良がおこりやすい欠点も有していた。
【0006】
また特公平5−80330号公報記載のトウプリプレグの製造方法では、トウ幅を広げた状態で樹脂を被覆しトウの相対する表面に皮膜を作り、そのトウをこねることで含浸させているが、この方法における含浸は扁平トウの表面に樹脂皮膜をつくり、次いで樹脂をトウ内に均一に押し込むことに主眼がおかれている。しかしながらこの方法ではまず均一な皮膜を実現することが問題となる。すなわちこの方法では、ドクターブレードとトウの隙間で塗布量を制御しているが、トウのかさばりや幅方向のトウ厚さは均等ではなく、しかも長手方向に変動するのでクリアランスが一定でも塗布厚さを精度よく制御することは至難である。更に混練ロールによるトウの混練でも厚さ方向への樹脂移動は起こりやすいが、横方向の樹脂移動が少ないため均一性が樹脂の塗布性に依存することになる。
【0007】
本発明は、上記従来の問題点を解決し、ホットメルト樹脂を用いて樹脂含有量を精密に制御し、且つ効率的な均一含浸を行うことによって高生産性でトウプリプレグ及びシート状プリプレグを製造し得る方法を提供するものである。
【0008】
【課題を解決するための手段】
本発明は、扁平にしたトウの少なくとも片面に樹脂を定量供給し、樹脂をトウに接触させると同時に又はその直後にトウの厚さ方向に浸透させ、トウ幅を狭める作用を有する手段とトウ幅を広げる作用を有する手段とを併用してトウを構成するフィラメントの横方向移動によりトウ内に樹脂を均一に含浸させ、その後冷却して巻取ることを特徴とするトウプリプレグの製造方法、及び上記トウプリプレグの製造方法において、扁平にしたトウを複数本用い、樹脂の接触、浸透、均一含浸及び冷却を行った後、各トウを分離せずにシート状に巻取ることを特徴とするシート状プリプレグの製造方法を要旨とするものである。
【0009】
また、本発明の実施態様は以下の通りである。すなわち、
(1)扁平にされたトウの少なくとも片面に樹脂を定量供給する前に、予めトウを加熱しておく。
(2)樹脂との接触時に規制される以上に予めトウ幅を拡げておき、樹脂との接触時にトウ幅を狭める。
(3)トウの樹脂付着量を樹脂吐出機の吐出量で制御する。
(4)トウに樹脂を接触させると同時に又はその直後に、トウの樹脂付着面を擦過させることにより樹脂をトウの厚さ方向に浸透させる。
(5)トウを構成するフィラメントの横方向移動を、さらに、トウの折り畳み、又はトウの加撚のうちの少なくとも一つの手段で行う。
(6)トウを構成するフィラメントの横方向移動による樹脂の均一含浸工程において、トウの走行速度未満の周速で回転する回転体にトウを接触させる。
(7)冷却工程において冷却ロール上でトウ幅を狭めると同時に圧縮してトウの断面形状を制御する。
(8)巻取る直前にトウ幅を狭めると同時に圧縮して断面形状を制御する。
(9)樹脂を均一に含浸した後、トウに粉体を付着させる。
(10)樹脂を均一に含浸した後、トウ片面にセパレーター担体を担持させる。
(11)扁平にした複数本のトウを用いて、樹脂の接触、浸透、均一含浸及び冷却を行った後、各トウを個別に巻取る。
【0010】
本発明におけるトウとは、無機繊維、有機繊維、金属繊維またはそれらの混合からなる強化用の長繊維(フィラメント)の束である。
無機繊維としては炭素繊維、黒鉛繊維、炭化珪素繊維、アルミナ繊維、タングステンカーバイド繊維、ボロン繊維、ガラス繊維等、有機繊維としてはアラミド繊維、高密度ポリエチレン繊維、その他一般のナイロン、ポリエステル等の有機繊維等が好適に用いられる。
また金属繊維としては、ステンレス、鉄等、フィラメント状になって移動性があれば使用可能である。
フィラメントの径は0.1μm以上100μm以下のものが好ましい。0.1μm未満ではフィラメントの強力が小さくフィラメントの横移動を起こす際に切断したり毛羽だまりが生じたりする問題があり、100μmを越えると硬くなりすぎて屈曲性に劣るので好ましくない。
【0011】
樹脂としては、繊維強化複合材料のマトリックス樹脂として用いられる熱硬化性樹脂及び熱可塑性樹脂が用いられ、例えば熱硬化性樹脂としては、エポキシ樹脂、フェノール樹脂、ビニルエステル樹脂、エポキシアクリレート樹脂、ウレタンアクリレート樹脂、フェノキシ樹脂、アルキド樹脂、ウレタン樹脂等を挙げることができ、また熱可塑性樹脂としては、PEEK、PEI、ポリアリレート、ポリスルフォン等の超エンジニアリングプラスチック、ナイロン、ポリエステル、ABS等のエンジニアリングプラスチック、さらにアクリル樹脂、ポリエチレン樹脂、ポリプロピレン樹脂等の汎用プラスチックを挙げることができる。
【0012】
これらの樹脂に必要な性状としては、含浸時における温度で流動性を有していることである。流動性の尺度としての粘度の範囲としては、1CPS(センチポアズ)以上100万CPS以下が好ましく、更に好ましくは、1CPS以上1万CPS以下である。その理由は、以下で説明するフィラメント移動による樹脂含浸作用でフィラメントの移動及びそれに伴う樹脂移動を容易にするために、少なくともフィラメント移動性は高くなければならず、そのためには樹脂の粘度を小さくしてフィラメント移動の抵抗を小さくする必要があるからである。
【0013】
粘度レベルにおいて1CPS未満の樹脂はほとんど存在せず、100万CPSを越える粘度ではフィラメント移動及びそれに伴う樹脂の移動がほとんど不可能である。またフィラー等の添加材の有無は含浸時に樹脂の流動性があれば問題はない。
【0014】
トウは扁平であることが樹脂との接触面積を広くするため望ましい。またトウ幅を一定幅にすることは定量供給した樹脂との接触面積を一定にする意味で重要である。一般的に強化繊維トウは一定幅になっていないので拡幅する必要がある。拡幅させる方法としては、円筒バーで擦過させる方法、振動を加える方法、及び押しつぶす方法等が挙げられる。本発明において、トウは該トウに樹脂が接触するときのトウ幅以上にインラインまたはオフラインで拡幅されていればよい。市販されているテープ状トウはオフラインで拡幅されたトウとみなされる。拡幅されているトウの幅は通常安定化しておらず、その広がり方にはばらつきがある。従って樹脂接触時に樹脂との接触面積を安定化させるには、樹脂接触直前あるいは樹脂接触時にトウ幅を狭めて安定化させることが効果的である。その方法の1例として、樹脂吐出口部又はその直前の位置に所定幅の溝を設けて、該溝内にトウを走行させてトウ幅を狭める方法が好適である。
【0015】
トウの予備加熱は、樹脂との接触後トウ内への樹脂の浸透時に樹脂温度が低下しないように、予めトウ温度を上昇させておく意味がある。予備加熱によりトウ温度を接触前の樹脂温度以上にしておけば、トウと樹脂の接触後のトウ温度は接触前の樹脂温度より低くなることはない。予備加熱方法としては加熱体との接触加熱、及び通電加熱、誘電加熱、赤外線加熱、雰囲気加熱等の非接触加熱法がいずれも使用可能である。
【0016】
トウに樹脂を定量供給させる方法としては、プランジャー式吐出機、ギアポンプ式吐出機、エクストルーダー等の溶融樹脂吐出機を用いるのが好ましく、特に超精密ギアポンプ又はエクストルーダーを用いるのが定量供給精度上理想的である。熱硬化性樹脂の場合で樹脂混合後の樹脂ライフが問題になるときは、硬化剤と主剤を別々に押し出しスタティックミキサー等で混合させながら供給すれば更に理想的である。付着の際に必要なことは樹脂が低粘度化してトウに付着しやすくなっていることである。
樹脂を過剰につけてダイス等で樹脂を絞り出し樹脂供給量を制御する方法があるが、ラインスピードが速くなるとダイス、トウ間の摩擦で糸切れ等をおこし易いので速い製造速度では問題である。
また特公平5−80330号公報に記載されているように、ドクターブレード等のクリアランスで制御する方法もあるが、樹脂の浸透しない基材上への塗布であれば基材に樹脂が浸透することがないので塗布厚さで付着量を制御できるが、トウでは浸透があるので精密に制御するのは難しく、またクリアランスにトウを通過させると糸切れ、詰まりの原因となりやすい。
【0017】
トウに含浸させる樹脂の含有量は10重量%以上80重量%以下が良い。10重量%未満では均一に含浸しにくく、80重量%を越えると複合材料成型品の機械特性に問題が生じる。機械特性の性能を効果的に発現させるには、30重量%以上50重量%以下が理想的である。
【0018】
本発明において、トウに樹脂を接触させると同時に又はその直後にトウの厚さ方向に樹脂を浸透させるのが、定量供給した樹脂をトウの中に遅滞なく浸透付着させる意味で重要である。この点でトウの両面に単に樹脂皮膜を形成するだけの特公平5−80330号の方法と著しく相違している。樹脂の具体的な浸透方法としては、樹脂を接触させたトウ面側をすばやく擦過するのが良い方法である。ここで擦過とは擦過体たとえば円弧上あるいはエッジ上でトウをこすることを意味する。
【0019】
擦過時にトウは擦過体側に押しつけられるので必然的にトウ厚さ方向への樹脂加圧力が働き、その結果樹脂がトウ内へ浸透する。トウは擦過体に押しつけられているので擦過体とトウの間には隙間は存在しない。擦過体との接触角は1°以上90°以下が望ましい。1°未満では樹脂浸透の効果は小さく、90°を越えると擦過による抵抗で張力が大きくなりすぎ糸切れを生じるおそれがある。擦過で急激な加圧力を発生させた場合、樹脂のトウ内への浸透は不均一となるが、ここでは均一に含浸させることを目的にしているわけではなく、樹脂の付着を確実にすることに主眼をおいている。従って、この樹脂含浸の均一化は次の含浸工程の重要課題となる。
【0020】
本発明の樹脂含浸工程におけるフィラメントの横方向移動は、トウに外力を加えてトウを構成するフィラメントを横方向(長手方向と直交する方向)に動かし、フィラメント間の相対位置を変化させて樹脂とフィラメントの接触機会を増すことにより、単なる加圧や毛細管現象による含浸効果以上の均一な含浸効果を上げることを特徴としている。具体的には、トウを折り畳む、トウ幅の拡大およびトウ幅の縮小の併用、又はトウを加撚する等の少なくとも一つの手段で行う。加撚手段によると樹脂がトウの外側に押し出される作用も付加される。
【0021】
これらの手段において、折り畳み手段と加撚手段は、幅縮小手段と同様にトウ幅を狭める傾向にある。そしてトウ幅を狭める作用を有する手段とトウ幅を拡大する手段とを併用すると均一含浸の効果が高くなる。
なお、加撚は樹脂含浸時におこなえばよく含浸後に撚りのない状態が必要なら含浸後に撚り戻しをすればよい。また仮撚りであれば撚り戻しをする必要はなく、撚りのないトウが必要な場合には望ましい。また加撚と同時にあるいは直後に擦過を加えればトウ幅の広がる傾向がでてきて、更に樹脂の厚さ方向の移動のため含浸の均一性は高くなる。
【0022】
フィラメントの横方向移動の均一含浸において、トウの走行速度未満の周速で回転する回転体にトウを接触させて擦過させることは、毛羽の堆積やロールのクリーニング等にとって有用である。擦過されていればトウは回転体表面で絡まりつくこともなく、また回転体はトウでこすられ且つ回転しているのでトウと接触する面は常にクリーニングされている状態となり、製造環境の向上にも有用である。なお回転体の周速はトウの走行速度未満であればよく、トウの走行方向と逆方向の回転であっても良い。
【0023】
樹脂を均一含浸させたトウは加熱により樹脂粘度が低くなっており、すぐには巻取れないので冷却して操作性を向上させる必要がある。冷却温度は樹脂が冷却体、たとえば冷却ロール表面に付着せず剥がれる温度であればよく、樹脂系に応じて冷却温度を決定する必要がある。たとえば通常のプリプレグ用として用いられる樹脂系においては常温で多少べたつきがあるため、0℃〜30℃の範囲内にトウ温度を下げるのが好ましい。
【0024】
本発明では、樹脂を均一含浸させたトウを溝付きロールやクリアランスを設けたロールで幅を狭めると同時に圧縮して断面形状を制御することができる。その制御位置は均一含浸後の冷却時又はボビンに巻取る直前が良い。ボビンに巻取る直前にトウが冷えすぎて断面形状賦型が難しい場合は賦型可能な温度に加熱した後断面形状を規制すればよい。
また断面形状制御はボビンに巻取った後、オフラインで行い再度巻き直すことも可能である。
【0025】
トウをボビンから引き出す時、トウの解舒性が重要となる。樹脂に常温で高粘度のものを使用した場合、トウ同士の接着は起こりにくく解舒も問題ないが、粘度が低いと解舒不能となる。それを解決する方法として粉体を表面に付着させ表面の粘着性をなくす方法がある。粉体の種類としては有機、無機の各種粉体が使用可能である。有機物質ではたとえば熱硬化性樹脂、熱可塑性樹脂が使用可能である。具体的には熱硬化性樹脂としてはエポキシ樹脂、フェノール樹脂などが良く、樹脂は硬化していても未硬化でもかまわない。熱可塑性樹脂としてはナイロン、ポリプロピレン、ポリエチレンなどが使用可能である。また無機物質ではタルク、シリカなど一般的なフィラーが使用可能である。
粉体を付着させる方法としてはいろいろとあるが、一般的には流動床中にトウを通過させる方法又は噴霧させる方法が良い。
粉体をトウに付着させる位置としては樹脂を均一に含浸させた後であればどこでも良い。
トウに粘着性がなくなり、ボビンからの解舒性が良好になれば、粉体の種類、粒子径、付着量には限定されない。
【0026】
トウのボビンからの解舒性を向上させる方法としては、セパレーター担体をトウ片面に担持させる方法も好適に用いられる。
担体としてはいろいろなものが使用可能であるが、トウとの剥離性がよくしかも材料費を低減化させるために安価なフィルム状のものがよい。典型的な例としてポリエチレンフィルム及びポリプロピレンフィルムが好適である。離型紙などでもよいが高価である。フィルムの幅はトウ幅程度のものであればよく、片面に担持させておけばボビンに巻取った後の解舒も良好である。
担持させる位置としては粉体付着と同様に樹脂を均一含浸させた後であればどこでもよいが、断面形状制御をおこなう場合は形状制御後が望ましい。
【0027】
複数本のトウプリプレグを個別に巻取って製造する場合は、複数本のトウに、樹脂の接触、浸透、均一含浸及び冷却を行った後、各トウを個別に巻取ればよい。樹脂の均一含浸はトウを複数本まとめて行っても、各トウを分離して個別に行ってもよい。ワインダーで巻取る際に分離されておればトウは個別に巻取ることができる。
また、複数本のトウからシート状のプリプレグを製造する場合は、扁平にした複数本のトウを用いて、樹脂の接触、浸透、均一含浸及び冷却を行った後、各トウを分離せずにシート状に巻取ればよい。この場合も、樹脂の均一含浸はトウを複数本まとめて行っても、各トウを分離して個別に行ってもよい。
【0028】
更に製造したプリプレグに更に撚りをかける必要があるなら適宜冷却前後に加撚工程をいれることができる。
ライン定速制御は原則的にどこで行ってもよいが、トウ冷却後又は樹脂付着前で行うのが望ましい。
ワインダーとしては、トウ状態で巻取る場合は市販のワインダーが使用可能である。
【0029】
本発明を図面に従って説明すると、図1は、トウプリプレグを製造するための基本的な工程の一例を示す側面図である。同図において、ボビンに巻かれてあるトウ2をクリール1から引き出し、引き出されたトウ2は擦過拡幅ロール3を通過させた後、ネルソンロール4で走行速度を制御しつつ供給する。樹脂加熱タンクとギアポンプを内蔵した樹脂吐出機5で樹脂を押し出し加熱管6を経由して吐出口7まで供給する。そのとき拡幅したトウ2を吐出口7部に設けた溝(図示せず)内に通して幅を狭め一定幅にして供給された樹脂と接触させる。その後樹脂浸透用擦過ロール8上で樹脂をトウ2の中に浸透させる。トウ幅を狭めるため、また樹脂付着や擦過による樹脂浸透の際に樹脂が溢れ出さないように樹脂浸透用擦過ロール8のトウ通過帯は溝状にするのが好ましい。その後フィラメント横方向移動含浸部9で均一含浸させ、均一含浸したトウ2は冷却ロール10で冷却される。冷却されたトウ2はトルクモーターロール12で定トルクで引き取り、最後にワインダー14でボビンに巻取る。
【0030】
図2は、トウを構成するフィラメントの横方向移動を、トウ幅の拡大と縮小とを併用して行う手段の一例を示す側面図で、同図において、15はトウ幅を拡大するためのロールであり、16はトウ幅を縮小するためのロールであって、ロールを傾斜させることによりトウ幅を狭めることができる。
【0031】
図3は、トウを構成するフィラメントの横方向移動を、トウの加撚とトウ幅の拡大とを併用して行う手段の一例を示す側面図で、同図において、17は加撚具を示している。
【0032】
図4は、トウを構成するフィラメントの横方向移動を、トウの折り畳みとトウ幅の拡大とを併用した手段の一例を示す側面図で、同図において、トウ2は折り畳みガイド19で徐々に折り畳まれて行き、垂直に立ったロール対18で完全に折り畳まれる。
【0033】
図5は、冷却ロール上でトウ幅を狭めると同時に圧縮してトウの断面形状を制御するための手段の一例を示す正面図で、同図において冷却ロール20に設けた凹部21と圧縮ロール22に設けた凸部とが適宜間隙をおいて嵌合し、その間にトウ2を通過させることにより、トウ幅を狭めると同時に圧縮してトウ2の断面形状を制御するようになっている。
【0034】
【実施例】
以下本発明を実施例により更に具体的に説明する。
【0035】
[実施例1]
図1に示す製造工程に、フィラメント横方向移動手段として図2に示す装置を2ユニット用いてトウプリプレグを製造した。トウとしてグラフィル社製炭素繊維TR30Gトウ1本を使用し、該トウ2を擦過拡幅ロール3で5mm幅以上に拡幅し、樹脂吐出口7部の溝で4mm幅に狭めてトウ2の片面に樹脂吐出口7から樹脂を供給接触させると共に樹脂浸透用擦過ロール8で擦過して樹脂をトウ2内に浸透させた。樹脂は油化シェルエポシキ社製エピコート1001及び834を50/50で混合し、その混合物にジシアンジアミドを4部混合した樹脂組成物を用いた。樹脂はタンクで65℃に保持され、ギアポンプから加熱ホース6を通して吐出口7から120℃で吐出した。吐出口7部近傍では樹脂のトウへの接触及びトウ内への浸透時に樹脂の溢れ出しや樹脂の停滞はなく、樹脂吐出機5から供給された樹脂が停滞なくトウに付着していることが確認された。
【0036】
その後図2のトウ幅拡大及び縮小ロール(いずれも回転させずに固定)間を通過させてトウを構成するフィラメントを横方向に移動させることによりトウ内に樹脂を均一に含浸させた。樹脂接触浸透後のトウ温度は70℃であったが、最初のロールで120℃までトウ温度を昇温させ、その後のロールでは樹脂温度は120℃に保持され、その時の粘度は約500CPSであった。最後のロールでトウ幅を約5mm幅に拡幅した後、次の冷却ロールでトウを冷却し、トルクモーターロール12で定トルクで引き取り、その後ワインダー14で巻取った。
トウプリプレグの製造速度は100m/minで含浸状態は良好であり、樹脂含有量は35%±1%の範囲内にあり高精度であった。
【0037】
[実施例2]
実施例1において、フィラメント横方向移動手段として図2に示す装置に代えて図3に示す装置を用いる他は、実施例1と同様にしてトウプリプレグを製造した。この場合の加撚具17による加撚数は10T/Mとした。
トウプリプレグの樹脂含浸状態は良好で樹脂含有量の精度も実施例1と同様に高精度であった。
【0038】
[実施例3]
実施例1において、フィラメント横方向移動手段として図2に示す装置に代えて図4に示す装置を用いる他は、実施例1と同様にしてトウプリプレグを製造した。
トウプリプレグの樹脂含浸状態は良好で樹脂含有量の精度も実施例1と同様に高精度であった。
【0039】
[実施例4]
実施例1の製造工程と同様の工程で、トウを5本用い、それぞれのトウをクリールから引き出して擦過拡幅ロールでそれぞれ5mm幅以上にした後4mm幅に狭め、次いで5本まとめて20mm幅にした後、樹脂吐出口からトウ片面に樹脂を供給接触させると共に樹脂浸透用擦過ロールで擦過して樹脂をトウ内に浸透させた。次いでトウを1本づつ分離し、トウ幅拡大及び縮小ロール間を通過させてトウを構成するフィラメントを横方向に移動させることにより樹脂をトウ内に均一に含浸させた。その後冷却ロールで冷却後、5台のワインダーで個別に巻取った。
得られた各トウプリプレグの樹脂含浸状態は良好で樹脂含有量の精度も実施例1と同様に高精度であった。
【0040】
[実施例5]
実施例1において、樹脂吐出口の前に加熱ロールを設置して、トウを予備加熱する以外は、実施例1と同様にしてトウプリプレグを製造した。
トウは加熱ロールとの接触で130℃に予備加熱した。吐出口から吐出した樹脂の温度は110℃であったが樹脂を接触、浸透させた後のトウ温度は約120℃となった。樹脂をトウ内に均一含浸させた後、冷却してボビンに巻取った。実施例1では樹脂接触、浸透後のトウ温度は予備加熱していなかったので最初のフィラメント横方向移動ロールでトウ温度を上昇させる必要があったが、樹脂接触前にトウを予備加熱して温度を上昇させておくことによりトウの加熱効率が向上した。
得られた各トウプリプレグの樹脂含浸状態は良好で樹脂含有量の精度も実施例1と同様に高精度であった。
【0041】
[実施例6]
実施例1においてトウ幅拡大及び縮小ロールを、周速約2.5m/分で回転させる以外は実施例1と同様にしてトウプリプレグを製造した。実施例1においては、トウ幅拡大及び縮小ロールの後部に毛羽が少し堆積していたが、本実施例では毛羽の堆積が全くなく、作業性が良好であった。
【0042】
[実施例7]
実施例1において、冷却ロール10の代わりに図5に示す凹部を有する冷却ロール20と凸部を有する圧縮ロール23を用いてトウ幅を狭めると同時に圧縮し、その後ワインダーに巻取って4mm幅の断面矩形のトウプリプレグを製造した。
【0043】
[実施例8]
実施例1において、ワインダーで巻取る直前に加熱ロールを用いてトウを加熱し、引き続いて図5に示す凹部を有する冷却ロール20と凸部を有する圧縮ロール23を用いてトウ幅を狭めると同時に圧縮し、その後ワインダーに巻取って4mm幅の断面矩形のトウプリプレグを製造した。
【0044】
[実施例9]
実施例1において、トウ構成フィラメントに樹脂を均一に含浸させた後、粉体の流動床を設置してトウに粉体を付着させ、その後トウを冷却して巻取りトウプリプレグを製造した。粉体には粒径約20μmのシリカ微粒子を用いた。粉体の付着量は約2重量%で、得られたトウプリプレグのボビンからの解舒性は良好であった。
【0045】
[実施例10]
実施例1において、トウ冷却後に5mm幅のポリプロピレンフィルムをトウの片面に担持させてワインダーに巻取った。得られたトウプリプレグのボビンからの解舒性は良好であった。
【0046】
[実施例11]
実施例7において、トウを10本用い、各トウを4mm幅の断面矩形のトウプリプレグとなした後、加熱ロールで加熱し、引き続いて図5に示す形状の40mm幅の凹部を有する冷却ロールの凹部内に並べると共に圧縮ロールの凸部で圧縮して40mm幅のシート状のプリプレグとなし、その片面にポリプロピレンフィルムを担持させてリールで巻取った。
得られたシート状プリプレグの樹脂含浸状態は良好で樹脂含有量の精度も実施例7のトウプリプレグと同様に高精度であった。
【0047】
【発明の効果】
本発明によれば、ホットメルト樹脂を用いて樹脂含有量を精密に制御し且つ効率的な均一含浸を行うことによって高生産性でトウプリプレグ及びシート状プリプレグを製造することができるという優れた効果を奏する。
【図面の簡単な説明】
【図1】本発明の基本的なトウプリプレグの製造工程の一例を示す側面図である。
【図2】トウを構成するフィラメントの横方向移動を、トウ幅の拡大と縮小とを併用して行う手段の一例を示す側面図である。
【図3】トウを構成するフィラメントの横方向移動を、トウの加撚とトウ幅の拡大とを併用して行う手段の一例を示す側面図である。
【図4】トウを構成するフィラメントの横方向移動を、トウの折り畳みとトウ幅の拡大とを併用して行う手段の一例を示す側面図である。
【図5】冷却ロール上でトウ幅を狭めると同時に圧縮してトウの断面形状を制御するための手段の一例を示す側面図である。
【符号の説明】
1 クリール
2 トウ
3 擦過拡幅ロール
4 ネルソンロール
5 樹脂吐出機
6 加熱管
7 吐出口
8 樹脂浸透用擦過ロール
9 フィラメント横方向移動樹脂含浸ロール
10 冷却ロール
11 ガイドロール
12 トルクモーターロール
13 ガイドロール
14 ワインダー
15 トウ幅拡大ロール
16 トウ幅縮小ロール
17 加撚具
18 垂直ロール
19 折り畳みガイド
20 冷却ロール
21 凹部
22 圧縮ロール
23 凸部
[0001]
[Industrial applications]
The present invention relates to a method for producing a tow prepreg used for a fiber reinforced composite material and a sheet prepreg (including a tape prepreg) comprising a plurality of tows.
[0002]
[Prior art]
The intermediate material used for the fiber-reinforced composite material is generally called a prepreg, and the reinforcing fiber tow is aligned on a hot melt film thinly coated with a resin on release paper, and a top film is placed on top of it. Alternatively, it is a general manufacturing method to stack a hot melt film from above, heat and / or press the resin to impregnate the constituent filaments of the reinforcing fiber tow with a resin, and then wind and manufacture.
As a typical example, JP-A-3-149230 and JP-B-4-5057 disclose a method of impregnating a resin by sandwiching the resin from above and below with a hot melt film.
[0003]
The method disclosed in the above-mentioned publication handles a large number of reinforcing fiber tows, and has a merit that it can be stably manufactured without contamination in the manufacturing process because it is wide and is sandwiched between protective films such as release paper.
Further, a method for producing a tow prepreg in which one tow is impregnated with a hot-melt resin is disclosed in Japanese Patent Publication No. 5-803330. In this method, a release paper or a hot-melt film is removed to produce a prepreg in tow units. Is the way.
[0004]
[Problems to be solved by the invention]
However, the prepregs manufactured by the methods disclosed in JP-A-3-149230 and JP-B-4-5057 have a very small variation in resin content when viewed in a wide direction in the width direction. When the width of the prepreg is small, the variation in the resin content is large, and when a prepreg manufactured in a wide width is cut into a narrow width and used, the variation in the resin content between the prepregs becomes too large. This is because strict control of the width of many tows is not possible, so even if the resin amount per unit area of the hot melt film is constant, there is a fluctuation in the amount of fibers per unit volume due to fluctuations in the spread of tow, The resin content per unit area after the resin impregnation (% by weight) fluctuates, and if the prepreg is used in a wide range, the resin content is offset and the accuracy is improved. For example, 1 to 5 wide prepregs are used. This is because when the slit tape is cut to a width corresponding to the degree of spread, or when about 1 to 5 tows are torn off from a wide prepreg to form a tow prepreg, the resin content greatly varies.
[0005]
Furthermore, regarding the resin impregnation speed, since the tows are placed side by side and pressed down from above and below by a protective sheet such as release paper, the movement of the filaments constituting the tow is almost impossible. Heating and pressing conditions from above and below, and if it is a thermosetting resin, it is determined in consideration of the life of the resin, and it is not necessary to simply lower the viscosity by heating, but it is a problem such as the length of the impregnation process etc. Therefore, there was a limit to the improvement of the production speed. Furthermore, when sandwiched between the hot melt films from above and below, air remains in the tow, so that impregnation failure tends to occur.
[0006]
In addition, in the method for manufacturing a tow prepreg described in Japanese Patent Publication No. 5-80330, a resin is coated in a state where the tow width is widened to form a film on the opposing surface of the tow, and the tow is impregnated by kneading. The impregnation in this method focuses on forming a resin film on the surface of the flat tow and then pushing the resin uniformly into the tow. However, this method has a problem in that a uniform film is first realized. In other words, in this method, the application amount is controlled by the gap between the doctor blade and the tow. However, since the bulk of the tow and the thickness of the tow in the width direction are not uniform and fluctuate in the longitudinal direction, even if the clearance is constant, the application thickness is constant. It is extremely difficult to control with high accuracy. Further, even when the tow is kneaded by the kneading roll, the resin moves in the thickness direction easily, but the uniformity depends on the resin coatability because the resin moves little in the lateral direction.
[0007]
The present invention solves the above-mentioned conventional problems, precisely controls the resin content using a hot melt resin, and performs efficient uniform impregnation to produce tow prepregs and sheet prepregs with high productivity. It provides a possible method.
[0008]
[Means for Solving the Problems]
The present invention provides a fixed amount of resin on at least one side of the flattened tow, and simultaneously or immediately after contacting the resin with the tow, penetrates in the thickness direction of the tow, Combining the means having the function of narrowing the tow width with the means having the action of expanding the tow width In the method for producing a tow prepreg, wherein the resin is uniformly impregnated in the tow by the lateral movement of a filament constituting the tow, and then cooled and wound, and the method for producing the tow prepreg, the flattened tow is used. Using a plurality of sheets, performing contact, permeation, uniform impregnation and cooling of the resin, and then winding each of the tows into a sheet without separating the tows. .
[0009]
The embodiments of the present invention are as follows. That is,
(1) Before the resin is quantitatively supplied to at least one side of the flattened tow, the tow is heated in advance.
(2) The tow width is increased in advance so as to be regulated at the time of contact with the resin, and the tow width is reduced at the time of contact with the resin.
(3) The amount of resin adhered to the tow is controlled by the amount of discharge of the resin discharger.
(4) Simultaneously with or immediately after the resin is brought into contact with the tow, the resin is penetrated in the thickness direction of the tow by rubbing the resin-attached surface of the tow.
(5) The lateral movement of the filament constituting the tow is further Of tow folding or tow twisting Performed by at least one means.
(6) In the step of uniformly impregnating the resin by moving the filaments constituting the tow in the lateral direction, the tow is brought into contact with a rotating body rotating at a peripheral speed lower than the running speed of the tow.
(7) In the cooling step, the cross-sectional shape of the tow is controlled by reducing the width of the tow on the cooling roll and simultaneously compressing the tow.
(8) Immediately before winding, narrow the tow width and simultaneously compress it to control the cross-sectional shape.
(9) After uniformly impregnating the resin, powder is attached to the tow.
(10) After uniformly impregnating the resin, the separator carrier is supported on one surface of the tow.
(11) Using a plurality of flattened tows, after performing contact, permeation, uniform impregnation and cooling of the resin, each tow is individually wound.
[0010]
The tow in the present invention is a bundle of reinforcing long fibers (filaments) composed of inorganic fibers, organic fibers, metal fibers, or a mixture thereof.
Inorganic fibers such as carbon fiber, graphite fiber, silicon carbide fiber, alumina fiber, tungsten carbide fiber, boron fiber, glass fiber, etc., and organic fibers such as aramid fiber, high density polyethylene fiber, and other general organic fibers such as nylon and polyester Etc. are preferably used.
As the metal fiber, stainless steel, iron, or the like can be used as long as it has a mobility in a filament form.
The diameter of the filament is preferably from 0.1 μm to 100 μm. If it is less than 0.1 μm, there is a problem that the strength of the filament is small and the filament may be cut or fuzzed when the filament is moved laterally. If it is more than 100 μm, it becomes too hard and inferior in flexibility, which is not preferable.
[0011]
As the resin, a thermosetting resin and a thermoplastic resin used as a matrix resin of the fiber-reinforced composite material are used. For example, as the thermosetting resin, epoxy resin, phenol resin, vinyl ester resin, epoxy acrylate resin, urethane acrylate Resins, phenoxy resins, alkyd resins, urethane resins, etc., and as the thermoplastic resin, super engineering plastics such as PEEK, PEI, polyarylate, polysulfone, engineering plastics such as nylon, polyester, ABS, and the like. General-purpose plastics such as acrylic resin, polyethylene resin and polypropylene resin can be used.
[0012]
The property required for these resins is that they have fluidity at the temperature at the time of impregnation. The range of viscosity as a measure of fluidity is preferably from 1 CPS (centipoise) to 1,000,000 CPS, more preferably from 1 CPS to 10,000 CPS. The reason is that, in order to facilitate the movement of the filament and the accompanying resin movement by the resin impregnation action by the filament movement described below, at least the filament mobility must be high, and for that purpose, the viscosity of the resin is reduced. This is because it is necessary to reduce the resistance of the filament movement.
[0013]
At a viscosity level less than 1 CPS of resin is scarcely present, and at viscosities above 1 million CPS, filament movement and consequent resin movement are almost impossible. The presence or absence of an additive such as a filler is not a problem as long as the resin has fluidity at the time of impregnation.
[0014]
It is desirable that the tow be flat to increase the contact area with the resin. It is also important to make the tow width constant so as to keep the contact area with the resin supplied in a constant amount constant. In general, the reinforcing fiber tow does not have a constant width, so it is necessary to increase the width. Examples of the method of widening include a method of rubbing with a cylindrical bar, a method of applying vibration, and a method of crushing. In the present invention, the tow may be expanded in-line or off-line beyond the tow width when the resin comes into contact with the tow. Commercially available taped tows are considered offline widened tows. The width of the widened tow is usually not stabilized, and its spread varies. Therefore, in order to stabilize the contact area with the resin at the time of the resin contact, it is effective to narrow the tow width immediately before or at the time of the resin contact to stabilize the area. As an example of the method, a method of providing a groove of a predetermined width at the resin discharge port or a position immediately before the resin discharge port and running the tow in the groove to reduce the tow width is preferable.
[0015]
Preheating the tow means that the tow temperature is raised in advance so that the resin temperature does not decrease when the resin permeates into the tow after contact with the resin. If the temperature of the tow is set to be equal to or higher than the resin temperature before the contact by the preheating, the tow temperature after the contact between the tow and the resin does not become lower than the resin temperature before the contact. As the preheating method, any of contact heating with a heating element, and non-contact heating methods such as electric heating, dielectric heating, infrared heating, and atmospheric heating can be used.
[0016]
As a method of supplying a fixed amount of resin to the tow, it is preferable to use a molten resin discharger such as a plunger discharger, a gear pump discharger, and an extruder. Particularly, it is preferable to use an ultra-precision gear pump or an extruder for the quantitative supply accuracy. Above ideal. When the resin life after mixing of the resins becomes a problem in the case of a thermosetting resin, it is more ideal if the curing agent and the main agent are separately extruded and supplied while being mixed by a static mixer or the like. What is necessary at the time of attachment is that the resin has a low viscosity and is easily attached to the tow.
There is a method of controlling the resin supply amount by squeezing the resin with a die or the like by excessively adding the resin. However, if the line speed is increased, the yarn is liable to be broken due to friction between the die and the tow.
Also, as described in Japanese Patent Publication No. 5-80330, there is a method of controlling the clearance with a doctor blade or the like. However, if the coating is performed on a substrate that does not penetrate the resin, the resin may penetrate the substrate. Since there is no toe, the amount of adhesion can be controlled by the coating thickness, but it is difficult to control precisely because the tow has permeation, and if the tow passes through the clearance, it can easily cause thread breakage and clogging.
[0017]
The content of the resin to be impregnated into the tow is preferably from 10% by weight to 80% by weight. If it is less than 10% by weight, it is difficult to uniformly impregnate it, and if it exceeds 80% by weight, problems occur in the mechanical properties of the composite material molded product. In order to effectively exhibit the performance of the mechanical properties, it is ideal that the content is 30% by weight or more and 50% by weight or less.
[0018]
In the present invention, it is important to allow the resin to penetrate the tow in the thickness direction of the tow at the same time as or immediately after the resin is brought into contact with the tow, from the viewpoint of allowing the resin to be quantitatively supplied to permeate into the tow without delay. In this point, the method is remarkably different from the method of Japanese Patent Publication No. Hei 5-80330, in which a resin film is simply formed on both surfaces of the tow. As a specific method of penetrating the resin, it is a good method to quickly rub the toe surface side with which the resin has contacted. Here, rubbing means rubbing the tow on a rubbing body such as an arc or an edge.
[0019]
Since the tow is pressed against the rubbing body at the time of rubbing, a resin pressing force inevitably acts in the thickness direction of the tow, and as a result, the resin permeates into the tow. Since the tow is pressed against the scraping body, there is no gap between the scraping body and the tow. The contact angle with the scraping body is desirably 1 ° or more and 90 ° or less. If it is less than 1 °, the effect of resin permeation is small, and if it exceeds 90 °, the tension due to the resistance due to abrasion becomes too large, and there is a possibility that the yarn breaks. When abrupt pressing force is generated by abrasion, the penetration of the resin into the tow becomes uneven, but here the purpose is not to impregnate the resin uniformly, but to ensure the adhesion of the resin The focus is on. Therefore, uniformization of the resin impregnation is an important issue in the next impregnation step.
[0020]
The lateral movement of the filament in the resin impregnation step of the present invention is performed by applying an external force to the tow to move the filament constituting the tow in the lateral direction (the direction perpendicular to the longitudinal direction), and changing the relative position between the filaments and the resin. By increasing the chance of contact with the filament, a more uniform impregnation effect than the impregnation effect due to simple pressurization or capillary action is achieved. Specifically, fold the toe, Combining toe width expansion and toe width reduction Or at least one means such as twisting the tow. According to the twisting means, the action of pushing the resin out of the tow is also added.
[0021]
In these means, the folding means and the twisting means tend to narrow the tow width similarly to the width reducing means. When the means for reducing the tow width and the means for expanding the tow width are used in combination, the effect of uniform impregnation is enhanced.
Note that twisting may be performed at the time of resin impregnation, and if untwisted state is required after impregnation, untwisting may be performed after impregnation. In the case of false twist, it is not necessary to perform untwisting, and it is desirable when a tow without twist is required. If abrasion is applied at the same time as or immediately after twisting, the tow width tends to widen, and the uniformity of impregnation increases due to the movement of the resin in the thickness direction.
[0022]
In the uniform impregnation of the lateral movement of the filament, contacting the tow with a rotating body rotating at a peripheral speed lower than the running speed of the tow and scraping the tow is useful for fuzz accumulation, roll cleaning, and the like. If rubbed, the tow does not become entangled with the surface of the rotating body, and the rotating body is rubbed and rotated by the tow, so that the surface that comes into contact with the tow is always cleaned, improving the manufacturing environment. Is also useful. It is sufficient that the peripheral speed of the rotating body is lower than the traveling speed of the tow, and the rotation may be in a direction opposite to the traveling direction of the tow.
[0023]
The tow uniformly impregnated with the resin has a low resin viscosity due to heating and cannot be wound immediately. Therefore, it is necessary to cool the tow to improve the operability. The cooling temperature may be a temperature at which the resin is peeled off without attaching to the surface of the cooling body, for example, the cooling roll, and it is necessary to determine the cooling temperature according to the resin system. For example, a resin system used for ordinary prepregs has some stickiness at room temperature, so it is preferable to lower the tow temperature within a range of 0 ° C to 30 ° C.
[0024]
In the present invention, the width of the tow uniformly impregnated with the resin can be reduced by a grooved roll or a roll provided with a clearance, and at the same time, the tow can be compressed to control the cross-sectional shape. The control position is preferably at the time of cooling after uniform impregnation or immediately before winding on a bobbin. If the tow is too cold just before winding on the bobbin and it is difficult to shape the cross-sectional shape, the cross-sectional shape may be regulated after heating to a temperature at which shaping is possible.
Further, the cross-sectional shape control can be performed off-line after winding on the bobbin, and re-winding.
[0025]
When pulling out the tow from the bobbin, the unwinding property of the tow is important. When a resin having a high viscosity at room temperature is used, adhesion between the tows does not easily occur and there is no problem in unwinding, but if the viscosity is low, unwinding is impossible. As a method for solving the problem, there is a method in which powder is adhered to a surface to eliminate stickiness of the surface. As the type of powder, various organic and inorganic powders can be used. As the organic substance, for example, a thermosetting resin or a thermoplastic resin can be used. Specifically, the thermosetting resin is preferably an epoxy resin, a phenol resin or the like, and the resin may be cured or uncured. As the thermoplastic resin, nylon, polypropylene, polyethylene and the like can be used. In addition, common fillers such as talc and silica can be used as the inorganic substance.
There are various methods for attaching the powder, but generally, a method of passing a tow through a fluidized bed or a method of spraying the tow is preferred.
The position where the powder adheres to the tow may be any position after the resin is uniformly impregnated.
As long as the tow loses adhesiveness and the unwinding property from the bobbin is improved, there is no limitation on the type, particle diameter, and amount of the powder.
[0026]
As a method for improving the unwinding property of the tow from the bobbin, a method of supporting a separator carrier on one side of the tow is also suitably used.
Although various carriers can be used, an inexpensive film-shaped carrier having good releasability from the tow and reducing material costs is preferable. As a typical example, a polyethylene film and a polypropylene film are suitable. Release paper may be used, but it is expensive. The width of the film may be about the width of the toe, and if it is held on one side, the unwinding after winding on a bobbin is also good.
The supporting position may be any position after the resin is uniformly impregnated as in the case of the powder adhesion. However, when controlling the cross-sectional shape, it is desirable after the shape control.
[0027]
In the case where a plurality of tow prepregs are individually wound and manufactured, the tows may be individually wound after contacting, permeating, uniformly impregnating, and cooling the plurality of tows. The uniform impregnation of the resin may be carried out collectively with a plurality of tows, or may be carried out separately from each tow. The tow can be individually wound if it is separated when wound by a winder.
Also, when manufacturing a sheet-shaped prepreg from a plurality of tows, using a plurality of flat tows, after contacting, infiltrating, uniformly impregnating and cooling the resin, without separating each tow What is necessary is just to wind up in a sheet form. In this case as well, the uniform impregnation of the resin may be performed by a plurality of tows collectively or by separating each tow separately.
[0028]
If it is necessary to further twist the produced prepreg, a twisting step can be appropriately performed before and after cooling.
Although the line constant speed control may be performed in principle anywhere, it is desirable to perform it after cooling the tow or before adhering the resin.
When winding in a tow state, a commercially available winder can be used as the winder.
[0029]
FIG. 1 is a side view showing an example of a basic process for manufacturing a tow prepreg. In FIG. 1, a tow 2 wound on a bobbin is pulled out of a creel 1, and the pulled out tow 2 is passed through a rubbing widening roll 3 and then supplied while controlling a traveling speed by a Nelson roll 4. The resin is extruded by a resin discharge machine 5 containing a resin heating tank and a gear pump, and supplied to a discharge port 7 via a heating pipe 6. At this time, the widened tow 2 is passed through a groove (not shown) provided in the discharge port 7 to make the width narrower and to make the width constant and to contact the supplied resin. Thereafter, the resin is made to penetrate into the tow 2 on the resin-penetrating rubbing roll 8. In order to reduce the tow width, and to prevent the resin from overflowing during resin penetration due to resin adhesion or rubbing, the tow passage band of the resin penetration rubbing roll 8 is preferably formed in a groove shape. Thereafter, the tow 2 is uniformly impregnated in the filament laterally moving impregnating section 9, and the uniformly impregnated tow 2 is cooled by the cooling roll 10. The cooled tow 2 is taken up by a torque motor roll 12 with a constant torque, and finally wound up on a bobbin by a winder 14.
[0030]
FIG. 2 is a side view showing an example of a means for performing the lateral movement of the filament constituting the tow by using both enlargement and reduction of the tow width. In FIG. 2, reference numeral 15 denotes a roll for enlarging the tow width. Reference numeral 16 denotes a roll for reducing the tow width, and the tow width can be reduced by inclining the roll.
[0031]
FIG. 3 is a side view showing an example of a means for performing the lateral movement of the filament constituting the tow by using both the twisting of the tow and the enlargement of the tow width. In FIG. ing.
[0032]
FIG. 4 is a side view showing an example of means for simultaneously moving the filament constituting the tow in the lateral direction by folding the tow and enlarging the tow width. In the drawing, the tow 2 is gradually folded by the folding guide 19. And is completely folded by the vertically standing roll pair 18.
[0033]
FIG. 5 is a front view showing an example of means for controlling the cross-sectional shape of the tow by simultaneously compressing and reducing the tow width on the cooling roll. In FIG. The tongue 2 is fitted with an appropriate gap, and the tow 2 is passed between the protrusions, thereby narrowing the tow width and simultaneously compressing the tow 2 to control the cross-sectional shape of the tow 2.
[0034]
【Example】
Hereinafter, the present invention will be described more specifically with reference to examples.
[0035]
[Example 1]
In the manufacturing process shown in FIG. 1, a tow prepreg was manufactured using two units of the apparatus shown in FIG. 2 as a filament lateral moving means. Using a single carbon fiber TR30G tow manufactured by Graphite Co. as a tow, the tow 2 is widened to a width of 5 mm or more with a rubbing widening roll 3, and is narrowed to a width of 4 mm with a groove at a resin discharge port 7 to form a resin on one surface of the tow 2. The resin was supplied from the discharge port 7 and brought into contact therewith, and was rubbed with the rubbing roll 8 for resin permeation to permeate the resin into the tow 2. The resin used was a resin composition in which Epicoat 1001 and 834 manufactured by Yuka Shell Eposiki were mixed at a ratio of 50/50, and 4 parts of dicyandiamide was mixed with the mixture. The resin was kept at 65 ° C. in a tank, and was discharged at 120 ° C. from a discharge port 7 through a heating hose 6 from a gear pump. In the vicinity of the discharge port 7, there is no overflow of the resin and no stagnation of the resin when the resin comes into contact with the tow and penetrates into the tow, and the resin supplied from the resin discharger 5 adheres to the tow without stagnation. confirmed.
[0036]
Thereafter, the resin was uniformly impregnated in the tow by passing between the tow width expanding and reducing rolls (fixed without rotating) in FIG. 2 to move the filaments constituting the tow in the lateral direction. Although the tow temperature after resin contact and infiltration was 70 ° C, the tow temperature was raised to 120 ° C on the first roll, and the resin temperature was maintained at 120 ° C on the subsequent rolls, at which time the viscosity was about 500 CPS. Was. After the width of the tow was increased to about 5 mm by the last roll, the tow was cooled by the next cooling roll, taken up by the torque motor roll 12 at a constant torque, and then wound by the winder 14.
The production speed of the tow prepreg was 100 m / min, the impregnation state was good, and the resin content was within the range of 35% ± 1%, and the precision was high.
[0037]
[Example 2]
A tow prepreg was manufactured in the same manner as in Example 1 except that the apparatus shown in FIG. 3 was used instead of the apparatus shown in FIG. In this case, the number of twists by the twisting tool 17 was 10 T / M.
The resin impregnation state of the tow prepreg was good, and the precision of the resin content was high as in Example 1.
[0038]
[Example 3]
A tow prepreg was manufactured in the same manner as in Example 1 except that the apparatus shown in FIG. 4 was used instead of the apparatus shown in FIG.
The resin impregnation state of the tow prepreg was good, and the precision of the resin content was high as in Example 1.
[0039]
[Example 4]
In the same process as the manufacturing process of Example 1, five tows were used, each tow was pulled out from the creel, and each was widened to 5 mm or more by a rubbing widening roll. After that, the resin was supplied and brought into contact with one side of the tow from the resin discharge port, and was rubbed with a rubbing roll for resin permeation so that the resin permeated into the tow. Next, the tows were separated one by one, and the filaments constituting the tow were moved laterally by passing between the tow width expanding and reducing rolls, so that the resin was uniformly impregnated in the tow. Then, after cooling with a cooling roll, it was individually wound up with five winders.
The resin impregnated state of each of the obtained tow prepregs was good, and the precision of the resin content was high as in Example 1.
[0040]
[Example 5]
A tow prepreg was manufactured in the same manner as in Example 1 except that a heating roll was installed in front of the resin discharge port to preheat the tow.
The tow was preheated to 130 ° C. by contact with a heating roll. Although the temperature of the resin discharged from the discharge port was 110 ° C., the tow temperature after contacting and permeating the resin was about 120 ° C. After the resin was uniformly impregnated in the tow, it was cooled and wound around a bobbin. In Example 1, since the tow temperature after resin contact and permeation was not preheated, it was necessary to raise the tow temperature with the first filament laterally moving roll. The heating efficiency of the tow was improved by raising.
The resin impregnated state of each of the obtained tow prepregs was good, and the precision of the resin content was high as in Example 1.
[0041]
[Example 6]
A tow prepreg was manufactured in the same manner as in Example 1, except that the tow width enlarging and reducing rolls were rotated at a peripheral speed of about 2.5 m / min. In Example 1, fluff was slightly deposited on the rear portion of the tow width expanding and reducing rolls. However, in this example, no fluff was deposited and the workability was good.
[0042]
[Example 7]
In the first embodiment, instead of the cooling roll 10, the tow width is reduced and compressed by using the cooling roll 20 having the concave portion and the compression roll 23 having the convex portion as shown in FIG. A tow prepreg having a rectangular cross section was manufactured.
[0043]
Example 8
In Example 1, the tow is heated using a heating roll immediately before winding by a winder, and subsequently, the tow width is reduced using a cooling roll 20 having a concave portion and a compression roll 23 having a convex portion shown in FIG. It was compressed and then wound up on a winder to produce a tow prepreg having a rectangular cross section with a width of 4 mm.
[0044]
[Example 9]
In Example 1, the resin was uniformly impregnated into the filaments of the tow, and then a fluidized bed of the powder was installed so that the powder adhered to the tow. Silica fine particles having a particle size of about 20 μm were used as the powder. The amount of powder adhered was about 2% by weight, and the obtained tow prepreg had good unwinding properties from the bobbin.
[0045]
[Example 10]
In Example 1, after cooling the tow, a polypropylene film having a width of 5 mm was supported on one surface of the tow and wound around a winder. The unwinding property of the obtained tow prepreg from the bobbin was good.
[0046]
[Example 11]
In Example 7, 10 tows were used, each tow was formed into a tow prepreg having a rectangular cross section having a width of 4 mm, and then heated with a heating roll. The sheet was arranged in the concave portion and compressed by the convex portion of the compression roll to form a 40 mm width sheet-shaped prepreg.
The resin-impregnated state of the obtained sheet-like prepreg was good, and the precision of the resin content was as high as that of the tow prepreg of Example 7.
[0047]
【The invention's effect】
Advantageous Effects of Invention According to the present invention, an excellent effect that tow prepregs and sheet prepregs can be produced with high productivity by precisely controlling the resin content using a hot melt resin and performing efficient uniform impregnation. Play.
[Brief description of the drawings]
FIG. 1 is a side view showing an example of a basic tow prepreg manufacturing process of the present invention.
FIG. 2 is a side view showing an example of a means for performing a lateral movement of a filament constituting the tow by using both enlargement and reduction of the tow width.
FIG. 3 is a side view showing an example of a means for performing a lateral movement of a filament constituting the tow by using both twisting of the tow and expansion of the tow width.
FIG. 4 is a side view showing an example of a means for performing a lateral movement of a filament constituting the tow by using both folding of the tow and enlargement of the tow width.
FIG. 5 is a side view showing an example of means for controlling the cross-sectional shape of the tow by compressing and simultaneously reducing the tow width on the cooling roll.
[Explanation of symbols]
1 Creel
2 toe
3 Abrasion widening roll
4 Nelson Roll
5 Resin discharging machine
6 heating tubes
7 Discharge port
8 Rubbing roll for resin penetration
9 Roller impregnated with resin moving laterally in filament
10 Cooling roll
11 Guide roll
12 Torque motor roll
13 Guide roll
14 Winder
15 Toe width enlargement roll
16 Toe width reduction roll
17 Twisting tool
18 vertical roll
19 Folding guide
20 Cooling roll
21 recess
22 Compression roll
23 convex

Claims (13)

扁平にしたトウの少なくとも片面に樹脂を定量供給し、樹脂をトウに接触させると同時に又はその直後にトウの厚さ方向に浸透させ、トウ幅を狭める作用を有する手段とトウ幅を広げる作用を有する手段とを併用してトウを構成するフィラメントの横方向移動によりトウ内に樹脂を均一に含浸させ、その後冷却して巻取ることを特徴とするトウプリプレグの製造方法。A fixed amount of resin is supplied to at least one side of the flattened tow, and at the same time or immediately after the resin is brought into contact with the tow, the resin is penetrated in the thickness direction of the tow, and a means having an action of narrowing the tow width and an action of expanding the tow width are provided. A method for producing a tow prepreg, characterized by uniformly impregnating the resin in the tow by laterally moving a filament constituting the tow in combination with a means having the tow, and then cooling and winding the tow. トウを構成するフィラメントの横方向移動として、さらに、トウの折り畳み又はトウの加撚により、トウを構成するフィラメントの横方向移動によりトウ内に樹脂を均一に含浸させ、その後冷却して巻取ることを特徴とする請求項1記載のトウプリプレグの製造方法。As the lateral movement of the filaments constituting the tow, furthermore, by folding the tow or twisting the tow, the resin is uniformly impregnated in the tow by the lateral movement of the filament constituting the tow, and then cooled and wound. The method for producing a tow prepreg according to claim 1, wherein 扁平にしたトウの少なくとも片面に樹脂を定量供給する前に、予めトウを加熱しておく請求項1または2記載のトウプリプレグの製造方法。The method for producing a tow prepreg according to claim 1 or 2, wherein the tow is heated in advance before a fixed amount of resin is supplied to at least one surface of the flattened tow. 樹脂との接触時に規制される以上に予めトウ幅を拡げておき、樹脂との接触時にトウ幅を所定幅に狭める請求項1〜3いずれか1項に記載のトウプリプレグの製造方法。The method for producing a tow prepreg according to any one of claims 1 to 3, wherein the tow width is increased in advance so as to be regulated at the time of contact with the resin, and the tow width is reduced to a predetermined width at the time of contact with the resin. トウの樹脂付着量を樹脂吐出機の吐出量で制御する請求項1〜4いずれか1項に記載のトウプリプレグの製造方法。The method for producing a tow prepreg according to any one of claims 1 to 4, wherein a resin adhesion amount of the tow is controlled by a discharge amount of the resin discharger. トウに樹脂を接触させると同時に又はその直後に、トウの樹脂付着面を擦過させることにより樹脂をトウの厚さ方向に浸透させる請求項1〜5いずれか1項に記載のトウプリプレグの製造方法。The method for producing a tow prepreg according to any one of claims 1 to 5, wherein the resin is made to penetrate in the thickness direction of the tow by rubbing the resin-attached surface of the tow simultaneously with or immediately after the resin is brought into contact with the tow. . トウを構成するフィラメントの横方向移動による樹脂の均一含浸工程において、トウの走行速度未満の周速で回転する回転体にトウを接触させる請求項1〜6いずれか1項にトウプリプレグの製造方法。The method for producing a tow prepreg according to any one of claims 1 to 6 , wherein the tow is brought into contact with a rotating body rotating at a peripheral speed lower than the running speed of the tow in the resin uniform impregnation step by laterally moving a filament constituting the tow. . 冷却工程において冷却ロール上でトウ幅を狭めると同時に圧縮してトウの断面形状を制御する請求項1〜7いずれか1項に記載のトウプリプレグの製造方法。The method for producing a tow prepreg according to any one of claims 1 to 7 , wherein in the cooling step, the cross-sectional shape of the tow is controlled by simultaneously reducing the tow width on a cooling roll and compressing the tow. 巻取る直前にトウ幅を狭めると同時に圧縮して断面形状を制御する請求項1〜8いずれか1項に記載のトウプリプレグの製造方法。The method for producing a tow prepreg according to any one of claims 1 to 8, wherein the cross-sectional shape is controlled by reducing the tow width and simultaneously compressing the tow just before winding. 樹脂を均一に含浸した後、トウに粉体を付着させる請求項1〜9いずれか1項に記載プリプレグの製造方法。The method for producing a prepreg according to any one of claims 1 to 9 , wherein a powder is adhered to the tow after uniformly impregnating the resin. 樹脂を均一に含浸した後、トウ片面にセパレーター担体を担持させる請求項1〜10いずれか1項に記載トウプリプレグの製造方法。The method for producing a tow prepreg according to any one of claims 1 to 10 , wherein the separator carrier is supported on one side of the tow after uniformly impregnating the resin. 扁平にした複数本のトウを用いて、樹脂の接触、浸透、均一含浸及び冷却を行った後、各トウを個別に巻取請求項1〜11いずれか1項に記載トウプリプレグの製造方法。The method for producing a tow prepreg according to any one of claims 1 to 11 , wherein the plurality of flat tows are used to perform contact, permeation, uniform impregnation and cooling of the resin, and then individually wind each tow. 請求項1〜12いずれか1項に記載のトウプリプレグの製造方法において、扁平にしたトウを複数本用い、樹脂の接触、浸透、均一含浸及び冷却を行った後、各トウを分離せずにシート状に巻取ることを特徴とするシート状プリプレグの製造方法。 The method for producing a tow prepreg according to any one of claims 1 to 12, wherein a plurality of flat tows are used, and after contact, permeation, uniform impregnation and cooling of the resin are performed, each tow is not separated. A method for producing a sheet-shaped prepreg, which is wound into a sheet.
JP21142694A 1994-09-05 1994-09-05 Method for producing tow prepreg and sheet prepreg Expired - Lifetime JP3571767B2 (en)

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