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JP7725968B2 - Method for manufacturing tape-shaped prepreg and method for manufacturing strip-shaped prepreg - Google Patents
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JP7725968B2 - Method for manufacturing tape-shaped prepreg and method for manufacturing strip-shaped prepreg - Google Patents

Method for manufacturing tape-shaped prepreg and method for manufacturing strip-shaped prepreg

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JP7725968B2
JP7725968B2 JP2021153307A JP2021153307A JP7725968B2 JP 7725968 B2 JP7725968 B2 JP 7725968B2 JP 2021153307 A JP2021153307 A JP 2021153307A JP 2021153307 A JP2021153307 A JP 2021153307A JP 7725968 B2 JP7725968 B2 JP 7725968B2
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shaped prepreg
tape
fiber
thermoplastic resin
fiber bundles
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JP2023045094A (en
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信彦 中切
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Toyobo MC Corp
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Description

本発明は、繊維強化熱可塑性樹脂成形品の原料となるテープ状プリプレグ、及び短冊状プリプレグの製造方法に関する。より詳細には、本発明は、製造装置において連続強化繊維の繊維束の糸道を安定させることにより、高い含浸性と生産性に優れた、物性ばらつきの少ないテープ状プリプレグ、及び短冊状プリプレグの製造方法に関する。 The present invention relates to a method for manufacturing tape-shaped prepregs and strip-shaped prepregs, which are used as raw materials for fiber-reinforced thermoplastic resin molded products. More specifically, the present invention relates to a method for manufacturing tape-shaped prepregs and strip-shaped prepregs that have high impregnation ability and excellent productivity, and little variation in physical properties, by stabilizing the fiber path of continuous reinforcing fiber bundles in the manufacturing equipment.

従来、複合材料のマトリックスには、熱硬化性樹脂が多く用いられてきた。しかし、貯蔵安定性、靭性、作業環境等の問題などから、近年、熱可塑性樹脂が注目され、開発が盛んに行われている。特に連続した強化繊維を使用する製造方法としては、例えば、強化繊維束中に微粉状の樹脂を含浸させたパウダー含浸法、マトリックス樹脂を繊維化して強化繊維と一緒に混繊させた混繊糸法、溶融樹脂を溜めた樹脂槽中に強化繊維を通過させることによって強化繊維中に含浸させる引抜成形法等がある。 Traditionally, thermosetting resins have often been used as the matrix for composite materials. However, due to issues such as storage stability, toughness, and working environment, thermoplastic resins have recently attracted attention and are being actively developed. Manufacturing methods that use continuous reinforcing fibers include, for example, the powder impregnation method, in which a finely powdered resin is impregnated into a reinforcing fiber bundle; the mixed fiber yarn method, in which the matrix resin is fiberized and mixed with the reinforcing fibers; and the pultrusion molding method, in which the reinforcing fibers are impregnated by passing them through a resin tank containing molten resin.

例えば特許文献1では、解舒機から引き出された繊維束を、幅方向に折れ曲がりやねじれを生じさせることなく繊維束を安定させて、所定の引き出し方向に収束させる繊維束の引き出し方法および装置について示されているが、含浸装置内における繊維束の糸道固定についての検討は無く、含浸装置を使用した生産機において十分に安定した生産ができない。 For example, Patent Document 1 describes a fiber bundle unwinding method and device that stabilizes the fiber bundle unwound from the unwinder without bending or twisting it in the width direction and converges it in a specified unwinding direction. However, there is no consideration of fixing the fiber bundle's yarn path within the impregnation device, and production machines using the impregnation device are unable to achieve sufficiently stable production.

特許文献2では、テープ状繊維束の搬送、案内する際に鍔付きロールなどで糸道を規制する場合には、繊維束の擦れ、折り畳まれの原因となり、それを回避するため、糸道と直角にねじれた位置に回転軸を有するガイドロールを有し、糸道の変動に対応して回転軸を糸道に対して傾けることにより、繊維束が本来の糸道位置に自動的に案内されるように構成された糸道ガイドである。しかし、特許文献1と同様、含浸装置内における繊維束の糸道固定についての記載が無く、かつ、複数の糸束同士における接触を避ける目的での糸道ガイドでは無いため、含浸装置を利用した機台における安定生産には不十分である。 Patent Document 2 describes a yarn guide that uses a flanged roll or similar device to restrict the yarn path when transporting and guiding a tape-shaped fiber bundle, which can cause the fiber bundle to rub and fold. To avoid this, the yarn guide has a guide roll with a rotation axis twisted at a right angle to the yarn path, and by tilting the rotation axis relative to the yarn path in response to fluctuations in the yarn path, the fiber bundle is automatically guided to its original yarn path position. However, like Patent Document 1, there is no mention of fixing the fiber bundle's yarn path within the impregnation device, and the yarn path guide is not designed to prevent contact between multiple yarn bundles, so it is insufficient for stable production on a machine using an impregnation device.

特許文献3、4は、箱状のチャンバー内に溶融樹脂を満たし、その装置中にて強化繊維を引き抜いて含浸させる装置について開示されている。その特徴は、含浸装置出口側に位置するノズル形状の工夫によって、機台の生産速度向上に伴うノズルでの繊維切れや、溶融樹脂の含浸レベルの低下を避けるための技術であり、含浸装置入口側にて繊維束の糸道固定についての記載はされていない。このため、含浸装置における繊維同士の接触に伴う繊維切れについての対策ではないため、安定生産のためには不十分である。 Patent documents 3 and 4 disclose equipment in which a box-shaped chamber is filled with molten resin, and reinforcing fibers are drawn out and impregnated within the equipment. A key feature of these equipment is the technology for preventing fiber breakage at the nozzle or a decrease in the impregnation level of the molten resin due to increased production speed of the machine, through the use of an ingenious nozzle shape located at the outlet of the impregnation equipment. However, there is no mention of fixing the fiber bundle thread path at the inlet of the impregnation equipment. Therefore, as this does not address fiber breakage due to contact between fibers in the impregnation equipment, it is insufficient for stable production.

特許第4332606号公報Patent No. 4332606 特許第4618132号公報Patent No. 4618132 特許第4872020号公報Patent No. 4872020 特許第5027929号公報Patent No. 5027929

上記の方法のうち、特に引抜成形方法では含浸装置にて連続強化繊維が通過する通路において、樹脂が強化繊維に被覆(含浸)される前の繊維束同士が接触する場合、繊維が擦れ合うことで損傷し、含浸装置の工程通過性が悪化する場合がある。経験的に、その傾向は、強化繊維が炭素繊維束の場合において顕著である。 Of the above methods, particularly with the pultrusion method, if fiber bundles come into contact with each other before they are coated (impregnated) with resin in the passage through which the continuous reinforcing fibers pass in the impregnation device, the fibers may rub against each other, causing damage and worsening the processability of the impregnation device. Empirically, this tendency is particularly pronounced when the reinforcing fibers are carbon fiber bundles.

本発明は、上記従来の課題を解決するためになされたものである。その目的とするところは、含浸性と生産性とを同時に満足させることである。強化繊維束同士の接触を回避し、高い工程安定性が得られることで、良好な繊維強化熱可塑性樹脂成形品用のテープ状プリプレグ、及び短冊状プリプレグの製造方法を提供することにある。 The present invention was made to solve the above-mentioned problems of the prior art. Its purpose is to simultaneously satisfy both impregnation properties and productivity. It aims to provide a method for producing tape-shaped prepregs and strip-shaped prepregs for excellent fiber-reinforced thermoplastic resin molded products by avoiding contact between reinforcing fiber bundles and achieving high process stability.

本発明者は、鋭意検討を行った結果、連続強化繊維(の繊維束)が通過する含浸装置の部品形状を工夫することで、熱可塑性樹脂が連続強化繊維に被覆(含浸)される前の連続強化繊維束同士が接触しないように改善した。具体的には、連続強化繊維が含浸工程の含浸前において接触する圧力が最も高まる位置において、糸道が固定されるように形状変更を行った。 After extensive research, the inventors have devised a component shape for the impregnation device through which the continuous reinforcing fiber (fiber bundles) pass, thereby preventing contact between the continuous reinforcing fiber bundles before they are coated (impregnated) with the thermoplastic resin. Specifically, the shape was changed so that the yarn path is fixed at the position where the pressure at which the continuous reinforcing fiber contacts the fibers before impregnation in the impregnation process is highest.

本発明は以下の通りである。
[1] 強化繊維と熱可塑性樹脂とを含有するテープ状プリプレグの製造方法であって、
連続強化繊維の繊維束を開繊する開繊工程、
開繊された連続強化繊維の繊維束を溶融した熱可塑性樹脂を含む槽に通して熱可塑性樹脂を含浸する含浸工程、及び、
熱可塑性樹脂を含浸した連続強化繊維の繊維束を賦形ローラーで潰し、冷却固化してテープ状プリプレグとする冷却固化工程、
を上記の順に有し、前記繊維束は複数本あり、前記含浸工程において、熱可塑性樹脂を含む槽までの間に繊維束同士が接触しない糸道安定化部品を有することを特徴とするテープ状プリプレグの製造方法。
[2] テープ状プリプレグに含有される強化繊維と熱可塑性樹脂との質量比(強化繊維/熱可塑性樹脂)が85/15~30/70である、[1]に記載のテープ状プリプレグの製造方法。
[3] 前記強化繊維がガラス繊維又は/及び炭素繊維である、[1]又は[2]に記載のテープ状プリプレグの製造方法。
[4] 前記糸道安定化部品が曲面ダイである、[1]から[3]のいずれかに記載のテープ状プリプレグの製造方法。
[5] 前記曲面ダイの上に、繊維束の進行方向に沿って、繊維束同士の接触を避けるための連続突起が設置されている、[4]に記載のテープ状プリプレグの製造方法。
[6] 前記連続突起の形状が半円状の断面形状である、[5]に記載のテープ状プリプレグの製造方法。
[7] [1]~[6]のいずれかに記載のテープ状プリプレグの製造方法において、得られたテープ状プリプレグをカッティングして短冊状プリプレグとするカッティング工程を有する短冊状プリプレグの製造方法。
[8] 前記短冊状プリプレグは、長さ5mm~100mm、幅4mm~60mm、厚み0.05mm~0.4mmである、[7]に記載の短冊状プリプレグの製造方法。
The present invention is as follows.
[1] A method for producing a tape-shaped prepreg containing reinforcing fibers and a thermoplastic resin,
a fiber-spreading step of spreading fiber bundles of continuous reinforcing fibers;
An impregnation step of passing the opened fiber bundle of continuous reinforcing fibers through a tank containing a molten thermoplastic resin to impregnate the thermoplastic resin; and
A cooling and solidifying process in which the fiber bundle of continuous reinforcing fibers impregnated with a thermoplastic resin is crushed with a shaping roller and cooled and solidified to form a tape-shaped prepreg;
a yarn path stabilizing part that prevents the fiber bundles from coming into contact with each other between the fiber bundles and a tank containing a thermoplastic resin in the impregnation step.
[2] The method for producing a tape-shaped prepreg according to [1], wherein the mass ratio of the reinforcing fiber to the thermoplastic resin contained in the tape-shaped prepreg (reinforcing fiber / thermoplastic resin) is 85/15 to 30/70.
[3] The method for producing a tape-shaped prepreg according to [1] or [2], wherein the reinforcing fibers are glass fibers and/or carbon fibers.
[4] The method for producing a tape-shaped prepreg according to any one of [1] to [3], wherein the yarn path stabilizing component is a curved die.
[5] The method for producing a tape-shaped prepreg according to [4], wherein continuous protrusions for preventing contact between fiber bundles are provided on the curved die along the traveling direction of the fiber bundles.
[6] The method for producing a tape-shaped prepreg according to [5], wherein the continuous projections have a semicircular cross-sectional shape.
[7] A method for producing a strip-shaped prepreg according to any one of [1] to [6], further comprising a cutting step of cutting the obtained tape-shaped prepreg into strip-shaped prepregs.
[8] The method for producing a strip-shaped prepreg according to [7], wherein the strip-shaped prepreg has a length of 5 mm to 100 mm, a width of 4 mm to 60 mm, and a thickness of 0.05 mm to 0.4 mm.

本発明によれば、含浸性と生産性とを同時に満足させ、連続強化繊維束同士の接触を回避することができる。そのことで、結果的に高い工程安定性が得られる。さらに、連続強化繊維束の糸道が安定化したことで、VF(繊維含有率)調整が容易となり、機台立ち上げ(生産開始)から生産品を採取するまでの時間が短縮され、VFが安定しない不良品の廃棄量も少なくなるという効果も有する。 The present invention simultaneously satisfies both impregnation and productivity requirements and prevents contact between continuous reinforcing fiber bundles. This ultimately results in high process stability. Furthermore, stabilizing the yarn path of the continuous reinforcing fiber bundles makes it easier to adjust the VF (fiber content), shortening the time from machine startup (start of production) to harvesting the finished product, and reducing the amount of defective products with unstable VF that are discarded.

実施例1と比較例1でそれぞれ用いた曲面ダイの模式図であり、Xは正面図、Yは正面図のA-Aの面、B-Bの面で切ったそれぞれの断面図、Zは曲面ダイの上部の斜視図である。1A and 1B are schematic diagrams of the curved dies used in Example 1 and Comparative Example 1, where X is a front view, Y is a cross-sectional view taken along the A-A plane and the B-B plane in the front view, and Z is a perspective view of the upper part of the curved die.

本発明における「テープ状プリプレグ」は、連続強化繊維と熱可塑性樹脂を含有する。「短冊状プリプレグ」は、強化繊維と熱可塑性樹脂を含有し、「テープ状プリプレグ」を短冊状にカットしたものである。テープ状プリプレグや短冊状プリプレグは、後工程にて予備成形体(シート状の成形体など)に成形後、所望の最終成形体(繊維強化熱可塑性樹脂成形品)に再成形可能である。 In this invention, the "tape-shaped prepreg" contains continuous reinforcing fibers and thermoplastic resin. The "strip-shaped prepreg" contains reinforcing fibers and thermoplastic resin and is a "tape-shaped prepreg" cut into strips. The tape-shaped prepreg and strip-shaped prepreg can be molded into a preform (such as a sheet-shaped molded product) in a subsequent process, and then remolded into the desired final molded product (fiber-reinforced thermoplastic resin molded product).

[強化繊維]
強化繊維は特に限定されないが、代表例としては、炭素繊維、炭化ケイ素繊維、ガラス繊維などの無機繊維、ボロン繊維などの金属繊維、アラミド繊維などの有機繊維が挙げられる。コスト、ならびに得られる成形品の弾性率および機械的強度の点から、ガラス繊維、炭素繊維などの無機繊維が好ましい。
[Reinforced fiber]
The reinforcing fibers are not particularly limited, but typical examples include inorganic fibers such as carbon fibers, silicon carbide fibers, and glass fibers, metal fibers such as boron fibers, and organic fibers such as aramid fibers. In terms of cost, and the elastic modulus and mechanical strength of the resulting molded product, inorganic fibers such as glass fibers and carbon fibers are preferred.

[熱可塑性樹脂]
熱可塑性樹脂は特に限定されないが、代表例としては、ポリアミド6、ポリアミド12、ポリアミド66、ポリアミド46などのポリアミド系樹脂、ポリエチレンテレフタレート、ポリブチレンテレフタレートなどのポリエステル系樹脂、ポリエチレン、ポリプロピレンなどのポリオレフィン系樹脂、ポリエーテルケトン樹脂、ポリフェニレンサルファイド樹脂、ポリエーテルイミド樹脂、ポリカーボネート樹脂などが挙げられる。これら熱可塑性樹脂は、変性されたものであっても良い。
[Thermoplastic resin]
The thermoplastic resin is not particularly limited, but typical examples include polyamide resins such as polyamide 6, polyamide 12, polyamide 66, and polyamide 46, polyester resins such as polyethylene terephthalate and polybutylene terephthalate, polyolefin resins such as polyethylene and polypropylene, polyether ketone resin, polyphenylene sulfide resin, polyetherimide resin, polycarbonate resin, etc. These thermoplastic resins may be modified.

特に好ましい熱可塑性樹脂の代表例は、以下の通りである。これらは、成形品の用途(または所望の特性)に応じて、適宜使用され得る。
(1)低コスト、成形時の流動性、耐水性、耐熱水性、または耐化学薬品性が要求される場合には、ポリオレフィン系樹脂が好ましい。入手が容易であるという理由で、ポリプロピレンが特に好ましく、本発明においては、酸変性されたポリプロピレンを用いることが好ましい。前述の強化繊維との接着性に特に優れるからである。
(2)耐摩耗性、耐油性、または長期耐熱特性が要求される場合には、ポリアミド系樹脂が好ましく、ポリアミド6、ポリアミド66、ポリアミドMXD6樹脂が特に好ましい。
(3)耐熱性、機械的強度、クリープ特性、耐薬品性、または耐油性が要求される場合には、ポリエステル系樹脂が好ましく、ポリエチレンテレフタレートが特に好ましい。
Representative examples of particularly preferred thermoplastic resins are as follows: These can be used as appropriate depending on the application (or desired properties) of the molded article.
(1) When low cost, fluidity during molding, water resistance, hot water resistance, or chemical resistance are required, polyolefin resins are preferred. Polypropylene is particularly preferred because of its easy availability, and in the present invention, it is preferable to use acid-modified polypropylene because it has particularly excellent adhesion to the reinforcing fibers described above.
(2) When wear resistance, oil resistance, or long-term heat resistance is required, polyamide resins are preferred, and polyamide 6, polyamide 66, and polyamide MXD6 resins are particularly preferred.
(3) When heat resistance, mechanical strength, creep characteristics, chemical resistance, or oil resistance are required, polyester resins are preferred, and polyethylene terephthalate is particularly preferred.

[開繊工程]
本発明は、連続強化繊維の繊維束を開繊する開繊工程を有する。開繊工程は、撚りが殆ど入らない状態で行われるのが望ましく、通常、ローラーおよび空気開繊工程が用いられるが、これに限定されるものではない。
[Opening process]
The present invention includes a fiber-opening step for opening a fiber bundle of continuous reinforcing fibers. The fiber-opening step is preferably carried out in a state where there is little twist, and typically, a roller or air-opening step is used, but is not limited thereto.

[含浸工程]
本発明は、開繊された連続強化繊維の繊維束を溶融した熱可塑性樹脂を含む槽に通して熱可塑性樹脂を含浸する含浸工程を有する。本発明で使用される含浸装置は、熱可塑性樹脂の融点以上の温度で、熱可塑性樹脂を溶融し充填した高圧の槽(以下、樹脂槽と称する場合もある)内にて、連続強化繊維に熱可塑性樹脂を含浸させるものである。
[Impregnation process]
The present invention includes an impregnation step in which a fiber bundle of opened continuous reinforcing fibers is passed through a tank containing molten thermoplastic resin to impregnate the fiber bundle with the thermoplastic resin. The impregnation device used in the present invention is a device for impregnating the continuous reinforcing fibers with the thermoplastic resin in a high-pressure tank (hereinafter sometimes referred to as a resin tank) filled with molten thermoplastic resin at a temperature equal to or higher than the melting point of the thermoplastic resin.

熱可塑性樹脂を連続的に効率よく含浸させるため、0.1MPa以上の圧力を有する樹脂槽を通すのが好ましい。0.1MPa未満である場合、含浸性が十分に得られにくくなる。樹脂槽内の圧力は高い方がより含浸性が向上し好ましく、より好ましくは0.3MPa以上、更に好ましくは、0.5MPa以上である。樹脂槽内の圧力は高い方がより含浸性が向上し好ましいが、設備コストも高くなるので、2MPa以下であることが好ましい。また、連続強化繊維が樹脂槽に入る前に、樹脂吐出スリットを有する曲面ダイに接触させる事が好ましい。樹脂吐出スリットから溶融させた熱可塑性樹脂を吐出させて、連続強化繊維の繊維束が曲面ダイに接触している側から熱可塑性樹脂の一部を含浸させることで、連続強化繊維が開繊された状態を保持したまま、プレ含浸が良好に行われ得るためである。 To ensure continuous and efficient impregnation with the thermoplastic resin, it is preferable to pass the material through a resin tank with a pressure of 0.1 MPa or more. If the pressure is less than 0.1 MPa, it will be difficult to achieve sufficient impregnation. A higher pressure in the resin tank improves impregnation, and is therefore preferred, more preferably 0.3 MPa or more, and even more preferably 0.5 MPa or more. A higher pressure in the resin tank improves impregnation, but this increases equipment costs, so a pressure of 2 MPa or less is preferred. It is also preferable to bring the continuous reinforcing fibers into contact with a curved die having a resin discharge slit before they enter the resin tank. By discharging molten thermoplastic resin from the resin discharge slit and impregnating a portion of the thermoplastic resin from the side where the continuous reinforcing fiber bundle is in contact with the curved die, pre-impregnation can be carried out satisfactorily while maintaining the continuous reinforcing fibers in an open state.

含浸装置前後には、連続強化繊維が通過する穴が設けられており、特に、含浸装置入口側の連続強化繊維の形状がテープ状プリプレグの含浸性に重要であることが経験的に知られている。具体的には、繊維間の樹脂浸透性を良好にするために繊維の開繊を良好にすること、本発明のように複数の繊維束により製造する場合には繊維束同士の重なりが少ないことが重要である。使用できる連続強化繊維の種類は特に限定はないが、当該含浸装置において製造する場合、繊維束同士の接触により損傷が著しい繊維種として炭素繊維がある。 There are holes before and after the impregnation device through which the continuous reinforcing fibers pass, and it is empirically known that the shape of the continuous reinforcing fibers at the inlet side of the impregnation device is particularly important for the impregnation of tape-shaped prepreg. Specifically, it is important to ensure good fiber spreading to improve resin penetration between the fibers, and when manufacturing using multiple fiber bundles as in this invention, it is important to minimize overlap between the fiber bundles. There are no particular restrictions on the type of continuous reinforcing fiber that can be used, but when manufactured using this impregnation device, carbon fiber is a type of fiber that is severely damaged by contact between fiber bundles.

含浸装置入口側において、熱可塑性樹脂が被覆していない状態における炭素繊維同士が接触すると、損傷が著しく、損傷した繊維が短繊維状の毛羽となり、含浸装置内に発生した炭素繊維の毛羽が蓄積される。含浸装置出口側からも、含浸装置内に蓄積された毛羽は順次排出されるが、排出量に比べて発生量が多い場合、含浸装置出口側の穴が閉塞すると同時に、その位置においてテープ状プリプレグが切断し操業停止となる。含浸装置入口側において、特に強化繊維が炭素繊維の場合、糸道を固定化して繊維束同士が接触しないようにすることが重要である。 When carbon fibers that are not coated with thermoplastic resin come into contact with each other at the entrance to the impregnation device, they are severely damaged, and the damaged fibers turn into short fiber fluff, which accumulates inside the impregnation device. The fluff that has accumulated inside the device is also gradually discharged from the exit side of the device, but if the amount of fluff generated is greater than the amount discharged, the hole on the exit side of the device will clog, causing the tape-shaped prepreg to break at that position and shutting down operations. At the entrance to the impregnation device, especially when the reinforcing fiber is carbon fiber, it is important to fix the yarn path to prevent fiber bundles from coming into contact with each other.

これまで、含浸装置入口側には、樹脂が被覆していない連続強化繊維の糸道を固定し調整するために、くし歯状のガイドを設置し、糸道を調整・固定化を行ってきた。生産開始前に含浸装置入口側の糸道をくし歯状ガイドにて調整完了しても、連続強化繊維を取付けた解舒機から繊維を含浸装置入口側に送り出すボビントラバース等の影響を受け、含浸装置入口側の繊維束の糸道は数mm単位で機台TD方向に振動する。そのため、特に連続強化繊維が炭素繊維の場合、含浸装置入口側において繊維束同士が接触しないように調整完了しても、操業経過に伴って繊維束同士が接触し、機台停止する場合が生じる。なお、繊維束同士の接触を回避するため繊維束を必要以上に離して糸道調整を行うと繊維束同士の接触リスクは下がるが、離した繊維束間から樹脂が漏れ出し、結果的に生産しているテープ状プリプレグの含浸性低下につながる。連続強化繊維に炭素繊維を選択した場合、繊維束同士が接触しない、近接した状態を保持したまま、糸道の固定化できることがテープ状プリプレグの品質安定も含めた機台操業性に非常に重要である。 Until now, comb-shaped guides have been installed at the entrance of the impregnation device to fix and adjust the yarn path of continuous reinforcing fibers that are not coated with resin. Even if the yarn path at the entrance of the impregnation device is adjusted using the comb-shaped guide before production begins, the yarn path of the fiber bundle at the entrance of the impregnation device vibrates in the TD direction of the machine by several millimeters due to the influence of the bobbin traverse that sends the fiber from the unwinder to which the continuous reinforcing fibers are attached to the impregnation device entrance. Therefore, especially when the continuous reinforcing fiber is carbon fiber, even if adjustments are completed to prevent fiber bundles from contacting each other at the entrance of the impregnation device, fiber bundles may come into contact with each other as the operation progresses, causing the machine to stop. Furthermore, adjusting the yarn path by spacing the fiber bundles farther apart than necessary to prevent contact between the fiber bundles reduces the risk of contact between the fiber bundles, but resin leaks between the separated fiber bundles, ultimately leading to reduced impregnation performance of the tape-shaped prepreg being produced. When carbon fiber is selected as the continuous reinforcing fiber, it is extremely important for machine operability, including the stable quality of the tape-shaped prepreg, that the fiber bundles are kept close together and the yarn path is fixed.

[糸道安定化部品]
具体的な方策として、含浸装置入口側で、糸道安定化部品を用いることが重要である。連続強化繊維の繊維束同士が接触しないように、連続強化繊維が含浸装置入口側において接触する圧力が最も高まる位置である曲面ダイにおいて、糸道が固定されるように糸道安定化部品を用いることが有効である。各繊維束が近接した状態で糸道が固定化されるように、曲面ダイの接糸部において機台MD方向(繊維束の進行方向)に、繊維束同士が接触するのを避ける凸状の突起(分離帯形状)を設けた。
[Thread path stabilizing parts]
As a specific measure, it is important to use a yarn path stabilizing component at the inlet side of the impregnation device. To prevent contact between the continuous reinforcing fiber bundles, it is effective to use a yarn path stabilizing component to fix the yarn path at the curved die, which is the position where the pressure at which the continuous reinforcing fibers come into contact at the inlet side of the impregnation device is highest. To fix the yarn path in a state where each fiber bundle is close to each other, a convex protrusion (separation zone shape) was provided in the machine machine direction (direction of travel of the fiber bundle) at the yarn contact part of the curved die to prevent contact between the fiber bundles.

突起の長さは、曲面ダイの接糸長(機台MD方向)にわたって、全長に設置されているのが好ましい。つまり、突起は繊維束の進行方向に沿って、繋がって設置された連続突起であることが好ましい。部分的に、あるいは点状に設置されている場合、局所的に連続強化繊維との接触圧が急激に高まり繊維の損傷につながる可能性がある。含浸装置に入る繊維束の数は、2本~5本であることが好ましく、曲面ダイに設置される連続突起は1本~4本であることが好ましい。 The length of the protrusions is preferably such that they are installed along the entire length of the curved die (machine machine direction). In other words, the protrusions are preferably continuous and installed along the direction of fiber bundle travel. If they are installed partially or in spots, the contact pressure with the continuous reinforcing fibers may increase suddenly in certain areas, potentially leading to fiber damage. The number of fiber bundles entering the impregnation device is preferably 2 to 5, and it is preferable that 1 to 4 continuous protrusions be installed in the curved die.

突起の高さは、特に規定はないが、各繊維束の糸道が確実に固定されれば良く、0.1mm~5mmが好ましい。高さが0.1mm未満であると糸道の固定化が難しく、5mmより高いと必要以上の高さでありオーバースペックである。さらに好ましくは、0.5mm~3mmの高さである。 There are no particular regulations regarding the height of the protrusions, but as long as the yarn path of each fiber bundle is securely fixed, a height of 0.1 mm to 5 mm is preferable. If the height is less than 0.1 mm, it will be difficult to fix the yarn path, and if it is more than 5 mm, it will be higher than necessary and will be over-specified. A height of 0.5 mm to 3 mm is even more preferable.

突起の断面は、特に限定されないが、開繊させたい繊維束を効率的に開繊させる必要がある。炭素繊維のような繊維同士の接触で損傷しやすい繊維の場合、断面形状に角があると接触圧が急激に高まり繊維の損傷につながる可能性があるため特に炭素繊維に対してはラウンド形状が好ましい。より具体的には上に凸の半円形状が好ましく、半径rが0.1mm~5mmが好ましい。半径rが0.1mm未満であると、糸道の固定化が難しく、半径が5mmより大きいと必要以上の幅と高さとなり、オーバースペックとなる。さらに好ましくは、半径rが0.25mm~1.50mmである。 The cross section of the protrusions is not particularly limited, but must efficiently spread the fiber bundles to be spread. For fibers that are easily damaged by contact with other fibers, such as carbon fiber, a round shape is preferable, especially for carbon fiber, because corners in the cross section can cause a sudden increase in contact pressure and lead to fiber damage. More specifically, an upwardly convex semicircular shape is preferable, with a radius r of 0.1 mm to 5 mm. If the radius r is less than 0.1 mm, it is difficult to fix the yarn path, and if the radius is more than 5 mm, the width and height will be greater than necessary, resulting in over-specification. Even more preferably, the radius r is 0.25 mm to 1.50 mm.

曲面ダイ上における一本の繊維束が通過する幅は、使用する強化繊維のフィラメント数によって左右されるが、3mm~30mmが好ましい。繊維束が通過する幅が3mmより狭い場合、曲面ダイ上で繊維束を集束することとなり繊維束への含浸性が不良となる。30mmより広いと、樹脂吐出スリットを有する曲面ダイでプレ含浸させた場合、繊維束両端からの樹脂漏れが生じる可能性がある。例えば12Kフィラメントの炭素繊維を使用する場合は、5mm~15mmが好ましい。 The width through which a single fiber bundle passes on the curved die depends on the number of filaments in the reinforcing fiber used, but is preferably 3 mm to 30 mm. If the fiber bundle passes narrower than 3 mm, the fiber bundle will be concentrated on the curved die, resulting in poor impregnation of the fiber bundle. If it is wider than 30 mm, resin leakage from both ends of the fiber bundle may occur when pre-impregnating using a curved die with a resin discharge slit. For example, when using 12K filament carbon fiber, a width of 5 mm to 15 mm is preferable.

以上のような最適形状化された突起を設置した曲面ダイを使用することで、含浸装置中における糸道を固定化することが可能となり、安定した品質のテープ状プリプレグや短冊状プリプレグを生産する事が可能となる。 By using a curved die equipped with optimally shaped protrusions as described above, it is possible to stabilize the yarn path in the impregnation device, making it possible to produce tape-shaped prepreg and strip-shaped prepreg of consistent quality.

[冷却固化工程]
本発明は、熱可塑性樹脂を含浸した連続強化繊維の繊維束を賦形ローラーで潰し、冷却固化してテープ状プリプレグとする冷却固化工程を有する。樹脂槽を通過した連続強化繊維は、引取張力により集束しやすく、この状態では連続強化繊維の細部に熱可塑性樹脂が含浸しきれていない。賦形ローラーで潰し冷却固化させることにより樹脂含浸性と、取り扱い性を向上させることができる。
[カッティング工程]
本発明は、テープ状プリプレグをカッティングして短冊状プリプレグとするカッティング工程を有する。カッティングは通常、ファンカッターで行われるが、特に限定はされない。
[Cooling solidification process]
The present invention includes a cooling and solidification process in which a fiber bundle of continuous reinforcing fibers impregnated with a thermoplastic resin is crushed with a shaping roller and cooled and solidified to form a tape-shaped prepreg. The continuous reinforcing fibers that have passed through the resin tank tend to be bundled due to the take-up tension, and in this state, the thermoplastic resin does not fully impregnate the fine parts of the continuous reinforcing fibers. Crushing with a shaping roller and cooling and solidifying can improve resin impregnation and handleability.
[Cutting process]
The present invention includes a cutting step of cutting the tape-shaped prepreg into strip-shaped prepreg. The cutting is usually performed using a fan cutter, but is not particularly limited thereto.

[テープ状プリプレグ]
テープ状プリプレグに含有される強化繊維と熱可塑性樹脂との質量比(強化繊維/熱可塑性樹脂)は、85/15~40/60である事が好ましい。強化繊維が、炭素繊維であり、熱可塑性樹脂がポリプロピレンである場合、この質量比を繊維体積含有率(Vf)で表すと、74%~25%となる。この質量比、繊維体積含有率は、短冊状プリプレグでも同様である。テープ状プリプレグのサイズは、長さは特に限定されず、幅4mm~60mm、厚み0.05mm~0.4mmが好ましい。
[Tape-shaped prepreg]
The mass ratio of the reinforcing fibers to the thermoplastic resin contained in the tape-shaped prepreg (reinforcing fibers/thermoplastic resin) is preferably 85/15 to 40/60. When the reinforcing fibers are carbon fibers and the thermoplastic resin is polypropylene, this mass ratio, expressed as a fiber volume content (Vf), is 74% to 25%. This mass ratio and fiber volume content are similar for strip-shaped prepregs. The size of the tape-shaped prepreg is not particularly limited in length, but a width of 4 mm to 60 mm and a thickness of 0.05 mm to 0.4 mm are preferred.

[短冊状プリプレグ]
生産されたテープ状プリプレグは、使用しやすいようにカッティングし、短冊状プリプレグとする。短冊状プリプレグのサイズは、長さ5mm~100mm、幅4mm~60mm、厚み0.05mm~0.4mmが好ましい。
[Strip-shaped prepreg]
The produced tape-shaped prepreg is cut into strip-shaped prepreg pieces for easy use. The strip-shaped prepreg preferably has a length of 5 mm to 100 mm, a width of 4 mm to 60 mm, and a thickness of 0.05 mm to 0.4 mm.

厚みが0.05mm未満であると生産効率が悪く、0.4mmを超えると含浸性が不足する傾向となる。厚みは、より好ましくは0.07mm~0.2mmの範囲内である。また幅は4mm未満、もしくは、60mmを超えると、後工程で予備成形体を生産する際に生産効率が悪くなる傾向がある。幅は、より好ましくは10mm~50mmの範囲である。長さに関しても5mm未満、若しくは100mmを超える場合、後工程で予備成形体を生産する際に生産性が悪くなる傾向がある。長さは、より好ましくは10mm~50mmの範囲内である。含有される強化繊維の質量比も85%を超えると樹脂含浸性が不十分となり破壊の起点となりやすく、40%未満の場合、強化繊維補強効果が得られにくくなる。強化繊維と熱可塑性樹脂のより好ましい質量比の範囲は、80/20~50/50である。この場合も、上記と同じVfは、66.7%~33.3%となる。 If the thickness is less than 0.05 mm, production efficiency is poor, and if it exceeds 0.4 mm, impregnation tends to be insufficient. The thickness is more preferably in the range of 0.07 mm to 0.2 mm. Furthermore, if the width is less than 4 mm or exceeds 60 mm, production efficiency tends to decrease when producing preforms in subsequent processes. The width is more preferably in the range of 10 mm to 50 mm. If the length is less than 5 mm or exceeds 100 mm, productivity tends to decrease when producing preforms in subsequent processes. The length is more preferably in the range of 10 mm to 50 mm. If the mass ratio of the reinforcing fibers contained exceeds 85%, resin impregnation becomes insufficient and they are likely to become the starting point of fracture. If it is less than 40%, the reinforcing fiber reinforcement effect is difficult to achieve. A more preferable range for the mass ratio of reinforcing fibers to thermoplastic resin is 80/20 to 50/50. In this case, the Vf, the same as above, is 66.7% to 33.3%.

また、テープ状プリプレグ、及び短冊状プリプレグは、必要に応じて、熱劣化防止剤、酸化劣化防止剤、紫外線吸収剤、などの添加剤を含有し得る。これらの添加剤の含有量は、目的に応じて変化し得るが、通常、テープ状プリプレグ、又は短冊状プリプレグの質量に対し、それぞれ0.5質量%以下が好ましく、より好ましくはそれぞれ0.2~0.5質量%の範囲内で添加される。 The tape-shaped prepreg and strip-shaped prepreg may also contain additives such as heat degradation inhibitors, oxidation degradation inhibitors, and UV absorbers, as needed. The amount of these additives added may vary depending on the purpose, but typically, the amount added is preferably 0.5% by mass or less, and more preferably 0.2 to 0.5% by mass, of the mass of the tape-shaped prepreg or strip-shaped prepreg.

以下、実施例により本発明を具体的に説明するが、本発明はこれらに限定されるものではない。 The present invention will be explained in detail below using examples, but the present invention is not limited to these examples.

(実施例1)
強化繊維として、連続炭素繊維の繊維束(東レ(株)製、TR700、800Tex、12,000f、巻長7,500m)を2本使用し、直径2cmのローラーに通し開繊後、0.6MPa以上の圧力を有する、溶融した酸変性されたポリプロピレン樹脂(アサヒテクノ工業(株)製、G2H、融点160℃)を含む240℃の樹脂槽を通し、樹脂を連続的に含浸させ、その後、賦形ローラーで潰し冷却固化させてテープ状プリプレグを得た後、カッティングし、炭素繊維66.7質量部にポリプロピレン33.3質量部(Vf=50%)が含浸されてなる、幅15mm、長さ35mm、厚み0.1mmの短冊状プリプレグを作製した。その際、樹脂槽直前に位置する、形状を工夫した曲面ダイを使用した。形状は、図1に示すように、各繊維束が近接した状態で糸道が固定化されるように、曲面ダイ接糸部において機台MD方向に繊維束同士が確実に固定されるように、凸状の突起(分離帯形状)Vを設けた。突起は、曲面ダイ接糸部の全長にわたって設置する連続突起とした。突起の断面は半円形状とした。半円形状は、半径0.5mmの半円形状であるため、高さ0.5mm、繊維束間の距離1mmの断面形状となる。また、炭素繊維束の1本あたりが曲面ダイ底面を通過する幅は9mmである。この曲面ダイは、樹脂吐出スリットを有するもので、樹脂吐出スリットから溶融させた前記の樹脂を吐出させて、連続炭素繊維の繊維束が曲面ダイに接触している側から樹脂の一部を含浸させること(プレ含浸)ができるようにした。なお、曲面ダイの前には、くし歯状の糸道固定ガイドが設置されており、糸道固定ガイドを使用して生産を行った。以下の評価を実施し、結果を表1に記す。
Example 1
Two continuous carbon fiber bundles (manufactured by Toray Industries, Inc., TR700, 800Tex, 12,000f, winding length 7,500m) were used as reinforcing fibers, and after passing through a 2 cm diameter roller and opening, the fibers were passed through a 240 ° C. resin tank containing molten acid-modified polypropylene resin (manufactured by Asahi Techno Industries Co., Ltd., G2H, melting point 160 ° C.) having a pressure of 0.6 MPa or more, and the resin was continuously impregnated, and then crushed with a shaping roller and cooled and solidified to obtain a tape-like prepreg. Then, the prepreg was cut and impregnated with 66.7 parts by mass of carbon fiber and 33.3 parts by mass of polypropylene (Vf = 50%). A strip-shaped prepreg having a width of 15 mm, a length of 35 mm, and a thickness of 0.1 mm was produced. At that time, a curved die with an devised shape located just before the resin tank was used. As shown in Figure 1, the shape of the curved die was such that the fiber bundles were closely spaced and the yarn path was fixed, and convex protrusions (separation zone shapes) V were provided to securely fix the fiber bundles to each other in the MD direction of the machine frame at the curved die contact area. The protrusions were continuous protrusions installed over the entire length of the curved die contact area. The cross section of the protrusions was semicircular. The semicircular shape had a radius of 0.5 mm, resulting in a cross-sectional shape with a height of 0.5 mm and a distance between fiber bundles of 1 mm. The width through which each carbon fiber bundle passed through the bottom surface of the curved die was 9 mm. This curved die had a resin discharge slit, through which the molten resin was discharged, allowing the continuous carbon fiber bundles to be partially impregnated with the resin from the side in contact with the curved die (pre-impregnation). A comb-shaped yarn path fixing guide was installed in front of the curved die, and production was carried out using the yarn path fixing guide. The following evaluations were performed, and the results are shown in Table 1.

(操業停止回数)
1ロット(連続炭素繊維7,500m分)生産中、連続炭素繊維の繊維束又はテープ状プリプレグの切断により、操業を停止した回数を数えた。
(繊維束からの樹脂漏れ)
曲面ダイとして連続突起を有さない曲面ダイを用いた比較例1では、曲面ダイ上の繊維束の間から漏れる樹脂量は多かった。曲面ダイ上に漏れる樹脂量が、比較例1より大幅(半分量以下)に減少した場合、「少ない」、比較例1と同程度の場合、「多い」とした。
(生産品採取までの時間)
機台の立ち上げから、生産品(短冊状プリプレグ)採取開始までの時間(分)を測定した。
(基材樹脂ロス率)
下記の式で、ロス率(%)求めた。
{(使用した熱可塑性樹脂の質量-採取した生産品中の熱可塑性樹脂の質量)/(使用した熱可塑性樹脂の質量)}×100
(基材繊維ロス率)
下記の式で、ロス率(%)求めた。
{(使用した強化繊維の質量-採取した生産品中の強化繊維の質量)/(使用した強化繊維の質量)}×100
(Number of shutdowns)
During the production of one lot (7,500 m of continuous carbon fiber), the number of times the operation was stopped due to breakage of the fiber bundle of continuous carbon fiber or the tape-shaped prepreg was counted.
(Resin leakage from fiber bundle)
In Comparative Example 1, in which a curved die having no continuous protrusions was used as the curved die, a large amount of resin leaked from between the fiber bundles on the curved die. If the amount of resin leaking onto the curved die was significantly reduced (half or less) compared to Comparative Example 1, it was rated as "small," and if it was about the same as Comparative Example 1, it was rated as "large."
(Time until product is harvested)
The time (minutes) from the start of the machine to the start of production of the product (strip-shaped prepreg) was measured.
(Base resin loss rate)
The loss rate (%) was calculated using the following formula:
{(mass of thermoplastic resin used−mass of thermoplastic resin in sampled product)/(mass of thermoplastic resin used)}×100
(Base fiber loss rate)
The loss rate (%) was calculated using the following formula:
{(mass of reinforcing fibers used−mass of reinforcing fibers in the collected product)/(mass of reinforcing fibers used)}×100

実施例1では、1ロット生産中、繊維束同士は近接した状態を保ちながら接触することなく、安定して生産することができた。併せて、後記する比較例1に比し、曲面ダイ上の繊維束間からの樹脂漏れも大幅に抑えられ、かつ、機台立ち上げ直後より早期に曲面ダイ上の糸道が安定するため、生産品採取までの時間が短縮され、基材樹脂ロス率、基材繊維ロス率が改善した。 In Example 1, the fiber bundles remained close to each other during the production of one lot, allowing for stable production without contact. Furthermore, compared to Comparative Example 1 described below, resin leakage from between the fiber bundles on the curved die was significantly reduced, and the yarn path on the curved die stabilized soon after the machine was started up, shortening the time until product collection and improving the base resin loss rate and base fiber loss rate.

(実施例2)
強化繊維/熱可塑性樹脂の質量比を57/43(Vf=40%)へ変更した以外は、実施例1と同法にて短冊状プリプレグを生産した。評価結果を表1に記す。実施例1と同程度の評価結果であった。
Example 2
A strip-shaped prepreg was produced in the same manner as in Example 1, except that the mass ratio of reinforcing fiber / thermoplastic resin was changed to 57 / 43 (Vf = 40%). The evaluation results are shown in Table 1. The evaluation results were similar to those of Example 1.

(実施例3)
強化繊維として、連続炭素繊維の繊維束(東レ(株)製、TR700、800Tex、12、000f、巻長7、500m)を2本と、あらかじめ繊維束1本あたりの繊度を約287Texに調整した連続ガラス繊維(日本電気硝子(株)製、約500f、巻長9.500m)2本を用意した。この繊度を調整した連続ガラス繊維束2本と連続炭素繊維束2本をそれぞれ解舒機から巻き出し、曲面ダイに入る前において曲面ダイの1レーンあたり連続炭素繊維束1本と連続ガラス繊維束1本を混繊させ1束とし、直径2cmのローラーに通し開繊後、0.6MPa以上の圧力を有する、溶融した酸変性されたポリプロプレン樹脂(アサヒテクノ工業(株)製、G2H、融点160℃)を含む240℃の樹脂槽を通過させて、強化繊維81質量部にポリプロピレン19質量部(Vf=50%[炭素繊維40%、ガラス繊維10%])が含浸されてなる、幅15mm、長さ35mm、厚み0.1mmの短冊状プリプレグを生産した。実施例1と同様に、樹脂槽直前に、形状を工夫した曲面ダイを使用し、実施例1と同様の手順で生産した。評価結果を表1に記す。実施例1と同程度の評価結果であった。
Example 3
As the reinforcing fibers, two fiber bundles of continuous carbon fiber (manufactured by Toray Industries, Inc., TR700, 800 Tex, 12,000 f, winding length 7,500 m) and two continuous glass fiber (manufactured by Nippon Electric Glass Co., Ltd., approximately 500 f, winding length 9,500 m) whose fineness per fiber bundle had been adjusted in advance to approximately 287 Tex were prepared. Two continuous glass fiber bundles and two continuous carbon fiber bundles with the adjusted fineness were unwound from the unwinder, and before entering the curved die, one continuous carbon fiber bundle and one continuous glass fiber bundle were mixed together per lane of the curved die to form one bundle. After passing through a 2 cm diameter roller and spreading, the bundle was passed through a 240 ° C. resin bath containing molten acid-modified polypropylene resin (manufactured by Asahi Techno Kogyo Co., Ltd., G2H, melting point 160 ° C.) having a pressure of 0.6 MPa or more, and passed through a resin bath at 240 ° C. containing 19 parts by mass of polypropylene (Vf = 50% [carbon fiber 40%; glass fiber 10%]). A strip-shaped prepreg having a width of 15 mm, a length of 35 mm, and a thickness of 0.1 mm was produced. As in Example 1, a curved die with an improved shape was used immediately before the resin bath, and production was carried out in the same manner as in Example 1. The evaluation results were similar to those of Example 1.

(実施例4)
実施例1において、曲面ダイ上の連続突起の断面形状を半円形状から四角状の物に変更した以外は、実施例1と同法にて短冊状プリプレグを生産した。曲面ダイの連続突起は、断面形状が四角形であり、高さ1mm、繊維束間1mmである。評価結果を表1に記す。
生産中、断面が半円形状の連続突起とした実施例1~3と同様、繊維束同士は近接した状態を保ちながら接触することはなかったが、断面形状が四角形で角があるため、繊維束が損傷し断続的に毛羽が発生した。そのため、発生した毛羽が含浸装置内に供給され、含浸ダイに蓄積された毛羽は順次含浸装置出口側から排出されるが、排出量に比べて曲面ダイからの毛羽発生量が多いため、含浸装置出口側の穴が閉塞し、テープ状プリプレグが切断する操業停止が1ロット中に2回発生した。それに伴い、基材樹脂ロス率、基材繊維ロス率ともに、実施例1~3に比較して多くなった。
Example 4
In Example 1, strip-shaped prepregs were produced in the same manner as in Example 1, except that the cross-sectional shape of the continuous protrusions on the curved die was changed from semicircular to rectangular. The continuous protrusions on the curved die had a rectangular cross-sectional shape, a height of 1 mm, and a fiber bundle spacing of 1 mm. The evaluation results are shown in Table 1.
During production, as in Examples 1 to 3, where the continuous protrusions had a semicircular cross section, the fiber bundles remained close to each other but did not come into contact with each other. However, because the cross section was square and had corners, the fiber bundles were damaged and fuzz was generated intermittently. As a result, the generated fuzz was fed into the impregnation device, and the fuzz accumulated in the impregnation die was sequentially discharged from the outlet side of the impregnation device. However, because the amount of fuzz generated from the curved die was greater than the amount discharged, the holes on the outlet side of the impregnation device clogged, causing the tape-shaped prepreg to break, resulting in two operational stoppages per lot. As a result, both the base resin loss rate and the base fiber loss rate were higher than in Examples 1 to 3.

(比較例1)
図1に示す、曲面ダイとして連続突起を有さない曲面ダイを用いた以外は、実施例1と同法にて短冊状プリプレグを生産した。曲面ダイの形状は、凸状の連続突起がなく、断面形状はフラットである。2本の繊維束が通る曲面ダイ底面の幅は20mmであり、それぞれの繊維束が通る糸道は、特に区分されていない状態である。なお、実施例1と同様、曲面ダイの前には糸道固定ガイドは使用した。評価結果を表1に記す。
曲面ダイ上の糸道を調整したにもかかわらず、繊維束同士の接触を十分回避できず、1ロット生産中に繊維束の接触が原因の強化繊維束切れにより、3回の機台停止を生じた。また、曲面ダイ上の繊維束からの樹脂漏れが絶え間なく生じること、機台の立ち上げから生産品採取までの時間を長く要することもあり、基材樹脂・繊維ロス率は実施例1に比較して大きいものとなった。
(Comparative Example 1)
A strip-shaped prepreg was produced in the same manner as in Example 1, except that a curved die without continuous protrusions, as shown in Figure 1, was used. The shape of the curved die was free of convex continuous protrusions and had a flat cross-sectional shape. The width of the bottom surface of the curved die through which the two fiber bundles passed was 20 mm, and the yarn paths through which each fiber bundle passed were not particularly separated. As in Example 1, a yarn path fixing guide was used in front of the curved die. The evaluation results are shown in Table 1.
Despite adjusting the yarn path on the curved die, contact between the fiber bundles could not be sufficiently avoided, and the machine stopped three times during the production of one lot due to breakage of the reinforcing fiber bundles caused by contact between the fiber bundles. In addition, resin leakage from the fiber bundles on the curved die occurred continuously, and it took a long time from starting up the machine to collecting the product, so the base resin and fiber loss rate was larger than in Example 1.

(比較例2)
強化繊維/熱可塑性樹脂の質量比を57/43(Vf=40%)へ変更した以外は、比較例1と同法にて短冊状プリプレグを生産した。評価結果を表1に記す。比較例1と同様、生産品採取までに曲面ダイ上の糸道を調整したにも関わらず、1ロット生産中に繊維束の接触が原因の強化繊維束切れにより、3回の機台停止を生じ、比較例1と同程度の評価結果であった。
(Comparative Example 2)
A strip-shaped prepreg was produced by the same method as in Comparative Example 1, except that the mass ratio of reinforcing fiber/thermoplastic resin was changed to 57/43 (Vf = 40%). The evaluation results are shown in Table 1. As in Comparative Example 1, even though the yarn path on the curved die was adjusted before the product was collected, the machine stopped three times during the production of one lot due to breakage of the reinforcing fiber bundles caused by contact between fiber bundles, and the evaluation results were similar to those of Comparative Example 1.

(比較例3)
強化繊維として、実施例3と同じものを用意した。曲面ダイとして比較例1で使用したものを用いた以外は、実施例3と同様に短冊状プリプレグを生産した。評価結果を表1に記す。混繊された異なる2種類の強化繊維が曲面ダイ上を通過するため、生産品採取開始までの糸道調整を丹念に調整したが、1ロット生産中に繊維束中の接触が原因の強化繊維束切れによる機台停止が5回生じた。そのため、基材ロス率は、比較例1、2に比較しても多い水準となった。
(Comparative Example 3)
The same reinforcing fibers as in Example 3 were prepared. Strip-shaped prepregs were produced in the same manner as in Example 3, except that the curved die used in Comparative Example 1 was used. The evaluation results are shown in Table 1. Because two different types of mixed reinforcing fibers passed over the curved die, careful adjustments were made to the yarn path before the start of product collection. However, during the production of one lot, the machine stopped five times due to breakage of the reinforcing fiber bundles caused by contact within the fiber bundles. As a result, the base material loss rate was higher than in Comparative Examples 1 and 2.

本発明によれば、テープ状プリプレグ、及び短冊状プリプレグ生産に際して引抜成形方法にて生産した場合、特に連続強化繊維を炭素繊維に選択した際に、繊維束同士を近接した状態を保ちながら接触することなく、安定して生産することができる。結果的に、高い含浸性を有する、物性ばらつきの少ない繊維強化熱可塑性樹脂であるプリプレグの製造方法が提供できる。 According to the present invention, when tape-shaped prepreg and strip-shaped prepreg are produced using the pultrusion molding method, particularly when carbon fiber is selected as the continuous reinforcing fiber, stable production is possible, with the fiber bundles kept close to each other but not in contact with each other. As a result, a method for producing prepreg, a fiber-reinforced thermoplastic resin with high impregnation properties and little variation in physical properties, can be provided.

V 突起 V protrusion

Claims (5)

炭素繊維を含む強化繊維と熱可塑性樹脂とを含有するテープ状プリプレグの製造方法であって、
連続強化繊維の繊維束を開繊する開繊工程、
開繊された連続強化繊維の繊維束を溶融した熱可塑性樹脂を含む槽に通して熱可塑性樹脂を含浸する含浸工程、及び、
熱可塑性樹脂を含浸した連続強化繊維の繊維束を賦形ローラーで潰し、冷却固化してテープ状プリプレグとする冷却固化工程、
を上記の順に有し、前記繊維束は複数本あり、前記含浸工程において、熱可塑性樹脂を含む槽までの間に繊維束同士が接触しない糸道安定化部品を有し、
前記糸道安定化部品が曲面ダイであり、
前記曲面ダイの上に、繊維束の進行方向に沿って、繊維束同士の接触を避けるための連続突起が設置されていることを特徴とするテープ状プリプレグの製造方法。
A method for producing a tape-shaped prepreg containing reinforcing fibers including carbon fibers and a thermoplastic resin,
a fiber-spreading step of spreading fiber bundles of continuous reinforcing fibers;
An impregnation step of passing the opened fiber bundle of continuous reinforcing fibers through a tank containing a molten thermoplastic resin to impregnate the thermoplastic resin; and
A cooling and solidifying process in which the fiber bundle of continuous reinforcing fibers impregnated with a thermoplastic resin is crushed with a shaping roller and cooled and solidified to form a tape-shaped prepreg;
in the above order, the fiber bundles are plural, and a yarn path stabilizing part is provided between the fiber bundles and a tank containing a thermoplastic resin in the impregnation step, so that the fiber bundles do not come into contact with each other,
The yarn path stabilizing component is a curved die,
A method for producing a tape-shaped prepreg, characterized in that continuous protrusions are provided on the curved die along the traveling direction of the fiber bundles to prevent contact between the fiber bundles .
テープ状プリプレグに含有される強化繊維と熱可塑性樹脂との質量比(強化繊維/熱可塑性樹脂)が85/15~30/70である、請求項1に記載のテープ状プリプレグの製造方法。 The method for producing tape-shaped prepreg according to claim 1, wherein the mass ratio of reinforcing fibers to thermoplastic resin (reinforcing fibers/thermoplastic resin) contained in the tape-shaped prepreg is 85/15 to 30/70. 前記連続突起の形状が半円状の断面形状である、請求項に記載のテープ状プリプレグの製造方法。 The method for producing a tape-shaped prepreg according to claim 1 , wherein the continuous projections have a semicircular cross-sectional shape. 請求項1~のいずれかに記載のテープ状プリプレグの製造方法において、得られたテープ状プリプレグをカッティングして短冊状プリプレグとするカッティング工程を有する短冊状プリプレグの製造方法。 4. The method for producing a tape-shaped prepreg according to claim 1 , further comprising a cutting step of cutting the obtained tape-shaped prepreg into strip-shaped prepregs. 前記短冊状プリプレグは、長さ5mm~100mm、幅4mm~60mm、厚み0.05mm~0.4mmである、請求項に記載の短冊状プリプレグの製造方法。 The method for producing a strip-shaped prepreg according to claim 4 , wherein the strip-shaped prepreg has a length of 5 mm to 100 mm, a width of 4 mm to 60 mm, and a thickness of 0.05 mm to 0.4 mm.
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JP2016078308A (en) 2014-10-16 2016-05-16 東洋紡株式会社 Manufacturing method of fiber reinforced thermoplastic resin molded article
JP2018515364A (en) 2015-04-30 2018-06-14 エボニック デグサ ゲーエムベーハーEvonik Degussa GmbH Method and apparatus for manufacturing fiber composite materials
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