JP2019001066A - Production method of long fiber reinforced thermoplastic resin filamentous material - Google Patents

Abstract

To provide a method which a physical property (Characteristic) of an obtained long fiber reinforced thermoplastic resin filamentous material can be made uniform by making uniform a degree of impregnation of a matrix resin and the like, and capable of continuously and stably producing a long object.SOLUTION: A tension of 5 to 100 g per one is applied to a reinforcing fiber bundle F via a tension adjusting means TC so that a surface temperature of the reinforcing fiber bundle F is a temperature range of Tm to Tm-200°C with respect to a temperature Tm of a molten thermoplastic resin while the thermoplastic resin is supplied to a crosshead die 2 by driving a melting extruder E. In a production method of long fiber reinforced thermoplastic resin filamentous material 100, the thermoplastic resin is partially impregnated into the separated each reinforcing fiber bundle F in the molten resin impregnated portion of a guide core and in a die, and subsequently through a convergent guide, is extruded and coated to a long fiber reinforcing fiber bundle group under pressure with a die having an extrusion nozzle of a predetermined sectional shape as a linear material.SELECTED DRAWING: Figure 1

Description

  The present invention relates to a method for producing a long fiber reinforced thermoplastic resin linear product comprising a long fiber bundle and a thermoplastic resin matrix.

Articles made of fiber reinforced thermosetting resin (hereinafter sometimes referred to as “FRP”) in which reinforcing fibers are bound with a synthetic resin are high in strength and light in weight, so that they can be used as an alternative to metal articles. It is used in many fields such as automobiles, electronics, agriculture and forestry, building materials and furniture. Pipes, rods, linear objects, etc. with long fiber bundles such as glass rovings, which are one of products using this FRP technology, as reinforcing fibers and thermosetting resin as a matrix have been used in various industrial fields for a long time. Yes.
In recent years, there is an increasing demand for using such long fiber reinforced resin long materials as individual members in products. In order to be able to be used as such an individual member, it is necessary that the elongate material can be shaped so as to conform to the shape of the product when the product to be used is processed. In particular, it is required that the target shape can be shaped and stabilized by temperature stimulation by heating.
However, in general, the FRP is completely impregnated with the thermosetting resin as the matrix resin up to the inside of the reinforcing fiber, and after curing, due to the characteristics of the thermosetting resin cured product, it is deformed by heating to a desired shape. It is difficult to perform plastic working. In particular, the FRP linear material in which the fibers are uniformly dispersed in the cross section in the longitudinal direction is very high in rigidity, is restored to a straight shape even when bent, and is not plastically deformed. Absent.

  On the other hand, an article made of a fiber reinforced thermoplastic resin in which a reinforcing fiber is impregnated with a thermoplastic resin (hereinafter sometimes referred to as “FRTP”) can be plastically deformed to some extent by heating. However, in a FRTP linear material in which a long fiber-like reinforcing fiber is impregnated with a thermoplastic resin as a matrix resin, bending by heat shaping is not always easy.

  In Patent Document 1, in a method for producing a long fiber reinforced composite material in which a molten thermoplastic resin is impregnated while drawing continuous reinforcing fibers, an excessive amount of resin is impregnated with a slit nozzle after impregnating or coating the fibers with the molten resin. A method for producing a long fiber reinforced composite material is disclosed, which is continuously drawn out while narrowing down and then adjusted to a desired shape through a shaping nozzle. And according to the manufacturing method of patent document 1, the dispersion | distribution of the fiber in the obtained composite material and the impregnation property of resin are also favorable, and the effect that a high quality composite material can be obtained stably stably is mentioned. ing.

  Patent Document 2 discloses a rope made of a carbon fiber reinforced composite material obtained by twisting a plurality of carbon fiber reinforced composite materials having a diameter of 1 to 5 mm in which a long fiber carbon fiber bundle is impregnated with a thermoplastic resin, and the production thereof. A method is disclosed. In Patent Document 2, since the melt viscosity of a thermoplastic resin is generally high, it is difficult to uniformly impregnate the resin into the carbon fiber bundle, but the thermoplastic resin is discharged at a constant rate with an extruder to impregnate the resin. A technique is disclosed in which resin is impregnated under pressure while a carbon fiber bundle is opened at a section, the fiber bundle is shaped into a circle with a die installed separately from an extruder, and wound with a winding device.

  Each of the methods for producing FRTP described in Patent Documents 1 and 2 has a problem of uniformly impregnating a molten thermoplastic resin into a long fiber-like reinforcing fiber bundle. There is no disclosure of heat shaping in a state bent in the direction.

  Patent Document 3 discloses a vehicle seat pad that includes a foam and a resin wire that is insert-molded into the foam and is locked by a locking portion of a seat skin material, and the resin wire includes a plurality of resin wires. A resin wire having a diameter of 1 to 5 mm is obtained by impregnating a thermoplastic resin into a long fiber having a thinned portion in which the resin is thinned in a bent portion. Has been. This resin wire is provided with a heat bending shapeability by bending the thermoplastic resin on the surface intermittently in the cross-sectional direction at a plurality of locations in a bent portion that is preliminarily assumed to be seat pad molding, The fiber inside the resin wire is exposed, and the exposed fiber is made to be bonded to the foam. However, since the exposed portion of the fiber is limited to the bent part, the entire resin wire is bonded to the foam. Sex itself was insufficient.

The present inventors have previously made a long-fiber-reinforced thermoplastic resin wire made of a long-fiber reinforcing material and a thermoplastic resin matrix, which is easy to bend in the longitudinal direction by heat shaping and easy to handle. The wire-reinforced thermoplastic resin linear product and its manufacturing method were studied intensively and filed as Japanese Patent Application No. 2006-148732.
The invention according to this application is a long fiber reinforcement having a cross-sectional sea-island structure composed of a sea portion made of a matrix resin, which is a thermoplastic resin, and three or more and 50 or less island portions made of a long-fiber reinforcing fiber bundle. In the thermoplastic resin wire, the reinforcing fiber bundle constituting the island portion has a non-impregnated portion not impregnated with the matrix resin in a cross section orthogonal to the longitudinal direction. The present invention relates to a resin linear material.

  Further, the present applicants previously described a long fiber reinforced thermoplastic resin linear material suitable for a vehicle seat as a vehicle sheet comprising a matrix resin that is a thermoplastic resin and a long fiber reinforcing fiber bundle. It is a long fiber reinforced thermoplastic resin linear material, and the reinforcing fiber bundle has a non-impregnated portion not impregnated with the matrix resin in a cross section orthogonal to the longitudinal direction, and a part of the reinforcing fiber bundle A long fiber reinforced thermoplastic resin linear material for vehicle seats, which is exposed on the surface of the linear object at discrete positions of 6 or more and 12 or less and continuous in the longitudinal direction of the linear object. A joint application was filed as Japanese Patent Application No. 2006-201598.

JP-A-5-147116 JP-A-5-33278 JP-A-2015-97596

The inventors of the present invention have studied the thermal formability of the long fiber reinforced thermoplastic resin linear material, and as a result, in the linear material having the sea-island cross section in the longitudinal direction, the matrix is formed between the long fiber reinforcing fibers. It has been confirmed that by forming a structure having an unimpregnated part without highly impregnating a thermoplastic resin as a resin, heat shaping is easy and shape forming processability is improved. Since the processability depends on the degree of impregnation of the matrix resin between the single fibers of the long fiber reinforcing fiber bundle, there may be variations between production lots, and there is a problem in quality stability and continuous productivity. It was.
Further, in the production of a long-fiber-reinforced thermoplastic resin linear material in which a part of the reinforcing fiber bundle is exposed on the surface of the linear material, and this exposed fiber can reinforce the bondability with a foam such as polyurethane. Therefore, it is necessary that the degree of exposure of the reinforcing fiber bundle on the surface and the degree of bonding between the reinforcing fiber bundle and the matrix resin constituting the linear object be within a certain range. There has been a demand for a method of reducing and stably producing.
The present invention relates to a method for producing a long fiber reinforced thermoplastic resin linear product comprising a matrix resin which is a thermoplastic resin and a fiber bundle for long fiber reinforcement, and a matrix which is a thermoplastic resin for a fiber bundle for long fiber reinforcement. To provide a method capable of making the physical properties (characteristics) of the obtained long fiber reinforced thermoplastic resin linear material uniform by uniformizing the degree of impregnation of the resin and the like, and capable of continuously producing a long product stably. Objective.

  In the method for producing a long fiber reinforced thermoplastic resin linear product comprising a matrix resin which is a thermoplastic resin and a long fiber reinforcing fiber bundle, the present inventors have provided a long fiber reinforcing fiber bundle having a predetermined number of twists. The tension is applied to the reinforcing fiber bundle via the tension adjusting means, and the reinforcing fiber bundle is heated to raise the temperature of the preheating device while heating the reinforcing fiber bundle. Guided to the head die, the molten resin impregnated (contact) portion of the guide core and the separated reinforcing fiber bundles in contact with the molten thermoplastic resin are brought into contact with each other, and the thermoplastic resin is put on each reinforcing fiber bundle. Including a step of partially impregnating and subsequently extruding and covering the long-fiber reinforcing fiber bundle group as a linear object under pressure with a die having an extrusion nozzle having a predetermined cross-sectional shape through a convergence guide, and the preheating Addition of reinforcing fiber bundle in the device Knowing that the object can be achieved by setting the surface temperature of the reinforcing fiber bundle to Tm to Tm-200 ° C. with respect to the temperature Tm of the molten thermoplastic resin. completed.

That is, the present invention provides the following [1] to [8].
[1] A method for producing a long fiber reinforced thermoplastic resin linear product comprising a matrix resin which is a thermoplastic resin and a long fiber reinforcing fiber bundle,
(1) A long-fiber reinforcing fiber bundle having a predetermined number of twists is drawn from a required number of creels through a tension adjusting means, and is passed through an unheated preheating device, and includes a separation guide, a molten resin impregnation portion, and a convergence guide. The fiber bundles are sequentially arranged and inserted through the predetermined through holes of the separation guide and the convergence guide of the guide core, the guide core is attached to the crosshead die main body, and then provided with a sheath core and an extrusion nozzle. A preliminary drawing step of a bundle of long fiber reinforcing fiber bundles, which is led to a die, a cooling tank, and a drawing device;
(2) While driving the take-up device and taking up the long fiber reinforcing fiber bundle group at a predetermined speed, the reinforcing fiber bundle is loaded with a tension of 5 to 100 g via the tension adjusting means. And driving the melt extruder while heating the reinforcing fiber bundle by heating the preheating device, supplying the thermoplastic resin to the crosshead die, and impregnating the guide core metal with the molten resin Each separated reinforcing fiber bundle is brought into contact with the molten thermoplastic resin in the part and die, and each reinforcing fiber bundle is partially impregnated with the thermoplastic resin, followed by a convergence guide, and a predetermined cross-sectional shape. A step of extruding and coating the long fiber reinforcing fiber bundle group as a linear object under pressure with a die having an extrusion nozzle of
(3) a step of cooling and solidifying the extrusion-coated linear material and taking it out;
Have
In the step of extrusion coating the linear material, the heating of the reinforcing fiber bundle in the preheating device is such that the surface temperature of the reinforcing fiber bundle is Tm to Tm-200 with respect to the temperature Tm of the molten thermoplastic resin. A method for producing a long fiber reinforced thermoplastic resin linear product, characterized in that the temperature reaches a range that reaches ° C.
[2] In the (2) extrusion coating step, the discharge hole portion of the extrusion nozzle 23 has a land L of 2 mm or more, and when the hole diameter is A, the extrusion nozzle is a cone having an upper base A toward the discharge side. The angle θ at which the frustoconical inclined line 232 and the discharge hole wall surface line 231 cross each other in the thickness direction cross section of the extrusion nozzle exceeds 90 °, and the opening at the tip of the opposing sheath core is cut out. The long fiber reinforced heat according to the above [1], wherein the molten thermoplastic resin is extrusion coated by a die having a sheath core having a relationship that the hole diameter B is 105 to 360% larger than the discharge portion hole diameter A. A method for producing a linear resin material.
[3] The convergent guide of the guide mandrel satisfies the following requirement (a) or the two requirements (a) and (b): [1] or [2] A method for producing a linear object.
(A) The hole diameter Dc of the central portion through hole of the convergence guide is 50 to 100% with respect to the outer diameter Dp of the long fiber reinforced thermoplastic resin linear material.
(B) The fan-shaped lower side diameter Dfc is twice the sector-shaped lower side radius forming the radial fan-shaped through hole of the convergence guide, and the sector-shaped lower side diameter Dfc is 105-105 with respect to the outer diameter Dp of the long fiber reinforced thermoplastic resin wire. The method for producing a long fiber-reinforced thermoplastic resin linear product according to [1] or [2], which is 360%.
[4] The long fiber reinforced thermoplastic resin linear material according to any one of [1] to [3], wherein a required number of the reinforcing fiber bundles are exposed on the surface of the linear material. Production method.
[5] The reinforcing fiber bundle is a multifilament in which fibers having a single fiber fineness of 1.5 to 30 dtex are bundled by 80 to 150 f and have a twist of 2 to 500 times / m. [1] The manufacturing method of the long fiber reinforced thermoplastic resin linear material of any one of-[4].
[6] The reinforcing fiber constituting the reinforcing fiber bundle is made of a thermoplastic resin, and the matrix resin is a thermoplastic resin having a melting point lower by 20 ° C. or more than the melting point or softening point of the reinforcing fiber, [1] A method for producing a long fiber-reinforced thermoplastic resin wire according to any one of [1] to [5].
[7] The reinforcing fiber composed of the thermoplastic resin is one or more kinds selected from polyethylene terephthalate fiber, polybutylene terephthalate fiber, polyethylene naphthalate fiber, polytrimethylene terephthalate fiber, polyacrylonitrile fiber, and aliphatic polyamide fiber. The method for producing a long fiber-reinforced thermoplastic resin wire according to [6], which is used in combination or in a mixed fiber.
[8] Any of the above [1] to [7], wherein the thermoplastic resin constituting the matrix resin is a polypropylene resin having a melt flow rate (230 ° C., 21.18 N) of 20 to 100 g / 10 min. 2. A method for producing a long fiber reinforced thermoplastic resin filament according to 1.

  According to the method for producing a long fiber reinforced thermoplastic resin linear material of the present invention, the degree of impregnation of the matrix resin, which is a thermoplastic resin, into the long fiber reinforcing fiber bundle and / or the degree of exposure of the required surface exposed fiber bundle is set. By adjusting, it is possible to provide a method capable of stably and continuously producing a long fiber reinforced thermoplastic resin linear material having uniform physical properties (characteristics) with good reproducibility.

It is explanatory drawing of the manufacturing process of the long fiber reinforced thermoplastic resin linear material of this invention. It is a schematic diagram of a loading type tensor as an example of the yarn tension adjusting means, (A) front view, (B) top view. It is a schematic diagram of the ironing type guide bar tensor as an example of the yarn tension adjusting means, (A) a front perspective view, (B) a top view. It is a schematic diagram of the tension measuring device of the reinforcing fiber bundle. It is explanatory drawing of the guides of the fiber bundle for long fiber reinforcement which comprises the guide core metal with which a crosshead die is mounted | worn, (B) The cross section which does not have a surface exposure fiber bundle by passing only through the central through-hole of a convergence guide It is a XX line broken sectional view of (A) separation guide, (B) convergence guide, and (C) convergence guide suitable when manufacturing a sea-island type long fiber reinforced thermoplastic resin linear material. It is explanatory drawing of the guides of the fiber bundle for long fiber reinforcement which comprises the guide core metal with which a crosshead die is mounted | worn, (B) By passing through the radial fan-shaped through-hole of a convergence guide, the required number of exposed fibers on the surface It is a XX line broken sectional view of (A) separation guide, (B) convergence guide, and (C) convergence guide which are suitable when manufacturing a long fiber reinforced thermoplastic resin linear thing which has a bundle. It is explanatory drawing of the guide core metal which hold | maintains the separation guide and convergence guide of the reinforcing fiber (bundle) used for this invention, (A) Sectional drawing of the half of a half-shaped guide core metal, (B) is ( The arrow view of A), (C) The front view of the half of a half-shaped guide mandrel, (D) is the side view of (C). The structure of the crosshead die of the melt extruder used in the present invention is shown, and the relationship between the hole diameter A of the discharge hole of the extrusion nozzle, the land length L, the angle θ, the hole diameter B of the opening at the tip of the sheath core, etc. FIG. It is explanatory drawing which shows the structure of the die | dye used for manufacture of the long fiber reinforced thermoplastic resin wire which has a required number of exposed fiber bundles on the surface of Example 2, (A) For long fiber reinforcement for an internal guide An explanatory view schematically showing a top view of the guide core bar through which the fiber (bundle) is inserted before being attached to the die, and (B) an explanatory view schematically showing a state where the guide core bar is attached to the die. C) It is explanatory drawing which shows typically the condition of the fiber bundle for reinforcement | strength in a die | dye, and the flow of matrix resin. It is explanatory drawing which shows typically the cross section of the long fiber reinforced thermoplastic resin linear material obtained by (A) Example 1 and (B) Example 2 of this invention, (C) is a line in (B) It is explanatory drawing, such as the degree of fiber exposure in the surface of a shaped object.

  Hereinafter, the manufacturing method of the long fiber reinforced thermoplastic resin linear material of this invention is demonstrated with reference to drawings. In the present invention, the drawings are for explaining the technical idea of the present invention, and the dimensional balance between the components and the members, the components, etc. are limited to those shown in the drawings. Never happen.

Regarding the method for producing a long fiber reinforced thermoplastic resin linear product of the present invention, first, the preliminary drawing step (1) will be described.
First, as schematically shown in FIG. 1, a long-fiber reinforcing fiber bundle F having a predetermined number of twists is pulled out from the required number of creels 1 and is not raised to the reinforcing fiber bundle via the tension adjusting means TC. The reinforcing fiber bundle group is drawn out from the hole of the guide core bar, the sheath core, and the extrusion nozzle that is passed through the warm preheating device PH, and the cooling extruder 3 is not filled with the cooling water. Then, a pre-drawing step (1) is performed in which the take-up device 4 such as a caterpillar type is held between the caterpillars and can be taken out.
The reinforcing fiber bundle may be passed through the guide mandrel 20 according to the following procedure.
7A and 7B, the reinforcing fiber bundles in predetermined holes of the separation guides 201a and 201b and the convergence guides 202a and 202b shown in FIG. F is set in the holding grooves 204 and 205 of each of the guides of the half-shaped guide mandrel 20 and combined with the half-shaped guide mandrel of the holding partner to form a cylindrical guide mandrel 20 assemble. Next, as illustrated in FIG. 9B in the case of manufacturing a linear object having the required number of exposed fiber bundles on the surface (Embodiment 2), the reinforcing fiber bundle F was passed through a predetermined hole. The guide mandrel 20 is fixed to the sheath core 21 fitted to the crosshead die portion 22 of the melt extruder, the reinforcing fiber bundle group is drawn from the tip of the hole of the extrusion nozzle 23, and is reinforced to the take-up device 4 as described above. Lead fiber bundle group.

Next, in the production method of the present invention, in the extrusion coating step of (2), the tension adjusting means is applied to the reinforcing fiber bundle F while the take-up device 4 is driven and the long fiber reinforcing fiber bundle group is taken up at a predetermined speed. A predetermined tension is applied through each TC, the preheating device PH is heated to drive the melt extruder E while heating the reinforcing fiber bundle, and the thermoplastic resin is supplied to the crosshead die 2. As shown in FIG. 9C, the reinforcing fiber impregnated portion 203 of the guide mandrel 20 and the separated reinforcing fiber bundles F in the die are brought into contact with the molten thermoplastic resin to thereby provide each reinforcing fiber. A bundle of thermoplastic resin is partially impregnated into the bundle, and then the fiber bundle group for reinforcing long fibers is linearized under pressure by the crosshead die 2 having the extrusion nozzle 23 having a predetermined cross-sectional shape through the convergence guide 202a or 202b. It is a process of extrusion coating as a product.
After the extrusion coating step (2), a continuous fiber-reinforced thermoplastic resin linear product is manufactured through (3) a step of cooling and solidifying the linear product that has been extrusion-coated and taking it out.
Further, in the method for producing a long fiber reinforced thermoplastic resin linear product of the present invention, in the step of extrusion coating the linear product, the heating of the reinforcing fiber bundle in the preheating device is performed by using a molten thermoplastic resin. The surface temperature of the reinforcing fiber bundle is in a range that reaches Tm to Tm−200 ° C. with respect to the temperature Tm.
Hereinafter, the manufacturing method of the long fiber reinforced thermoplastic resin linear material of the present invention will be described in more detail.

<Number of twists of fiber bundles for reinforcing long fibers, fiber configuration>
The fiber bundle for reinforcing long fibers used in the present invention needs to have a predetermined number of twists. In the case where the required number of reinforcing fibers are exposed on the surface of the linear object, if there is no twist, the portion of the fiber bundle where the fiber single yarn is not adhered to the matrix resin around it will fall off. To do. That is, there is a twist, that is, the fiber bundle is twisted at a predetermined helical pitch in the longitudinal direction, so that any one of the bottom of the matrix resin groove, the peripheral wall, etc. at a predetermined position to be exposed There is a high probability that the twisted monofilament will bite into the matrix resin side and so-called anchor adhesion. That is, the structure is such that the single yarn of the fiber appears on the outermost surface or bites into the matrix resin side so as not to fall off. The number of twists of the reinforcing fiber bundle is preferably 2 to 500 sweet twists per meter, and if there is a stronger twist than this, the familiarity and embedding of the matrix resin near the surface of the fiber bundle will deteriorate, The reinforcing fiber bundle exposed to the surface is likely to fall off, and the function as a linear object is also reduced. It is possible to use a reinforcing fiber bundle having no twist at all, but in this case, it is only necessary to generate a twist of 2 times / m or more and draw it out by feeding with a twist. In addition, when using the linear object by cutting it short, twisting of the length or less is necessary. For example, when using it by cutting to 200 mm, twisting is preferably performed once within 200 mm, preferably 3 times or more. I need it. In the commercially available reinforcing fiber bundle used for the reinforcing fiber, the polyethylene terephthalate (PET) fiber is twisted 50 times / m, the glass yarn is 40 times / m, and the aramid fiber is 0 times / m. With no twist.
Further, the reinforcing fiber bundle uses multifilaments in which fibers having a single fiber fineness of 1.5 to 30 dtex are bundled by 80 f to 150 f and have a twist of 2 to 500 times / m. However, there are no problems such as generation of cracks during withdrawal from the creel and difficulty in adjusting the non-impregnation rate of the matrix resin, and this is preferable from the viewpoint that a moderate reinforcing effect can be exhibited.

<Tension adjusting means for long fiber reinforcing fiber bundle>
In the above (2) extrusion coating step, the tension adjusting device used as a tension adjusting means for making the tension during running of the reinforcing fiber bundle constant can apply a constant tension to the reinforcing fiber bundle. If there is, it will not be specifically limited. For example, as shown in FIG. 2, the fiber bundle is passed between the two flat plates D having the axis J as shown in FIG. A device (loading type tensor) for adjusting the tension by loading the weight W on the upper surface of the flat plate, or two cylindrical guides GB standing on the circular plate as shown in FIG. By changing the contact angle θ with the fiber bundle F, a so-called “ironing type guide bar tensor” that can change the tension can be easily used. A combination of these may also be used.
In the extrusion coating step (2), the tension to the reinforcing fiber bundle is 5 to 100 g, more preferably 5 to 95 g, and particularly preferably 10 to 50 g. If the tension is less than 5 g, sagging occurs between the single fibers constituting the reinforcing fiber bundle in the manufacturing process, and the continuous production is hindered by being entangled at the entrance of the guides or in the worst case. Further, if it exceeds 100 g, the molten fiber impregnated portion 203 and the die of the guide core bar are difficult to impregnate the molten thermoplastic resin into the reinforcing fiber bundle, and the long fiber reinforced thermoplastic resin linear material has a low reinforcing effect by the fibers. In addition, when a surface-exposed type linear object is intended, since the fiber bundle is not exposed on the surface of the linear object, there is a problem that a locking force with the foam does not appear in insert molding or the like. Arise.

<Preheating of reinforcing fiber bundle>
In the production method of the present invention, in the step of extrusion-coating the linear product of (2), the reinforcing fiber bundle is heated in the preheating device with respect to the temperature Tm of the molten thermoplastic resin. It is necessary to make the surface temperature of the bundle reach Tm to Tm-200 ° C. The preheating device PH to be used is preferably an electrical device from the viewpoint of ease of temperature control, safety, and the like. In the preliminary drawing step, the guide operation of the reinforcing fiber bundle to the separation guide of the reinforcing core, the convergence guide It is preferable that the structure can be opened to the lower half and the upper half in view of the sorting operation of the fiber bundle for embedding the linear object in the predetermined hole and the fiber bundle for exposure. The heating method may be any of hot air, far infrared heater, and the like. In the case of using the hot air type, it is preferable that the direction of the hot air is made to follow the traveling direction of the reinforcing fiber bundle from the viewpoint that the disturbance of the fiber bundle hardly occurs.

In the step (2), that is, in the step of extrusion-coating the long fiber reinforcing fiber bundle group as a linear product, the heating of the reinforcing fiber bundle in the preheating device is performed with respect to the temperature Tm of the molten thermoplastic resin. By setting the surface temperature of the reinforcing fiber bundle to a range that reaches Tm to Tm-200 ° C., when the reinforcing fiber bundle and the matrix thermoplastic resin are brought into contact with each other, the thermoplastic resin is partially added to each reinforcing fiber bundle. It is possible to impregnate, and the obtained long fiber reinforced thermoplastic resin linear material can have predetermined characteristics. That is, if it demonstrates with FIG. 9, the surface temperature of the reinforcing fiber bundle F reaches Tm-Tm-200 degreeC at the time of the reinforcing fiber bundle F driving | running the molten resin impregnation part 203 of the guide metal core 20. FIG. Must be in range. For example, if the surface temperature of the reinforcing fiber bundle F is fed to the guide core 20 at room temperature, not only does the familiarity with the matrix resin worsen, but the temperature of the matrix resin around the fiber bundle F also decreases. If the melt viscosity becomes high, troubles such as fiber breakage may occur and continuous production may become impossible. Once the fiber breakage occurs, it is necessary to clean the resin reservoir in the crosshead 2 and then pass the fiber bundle F again, resulting in a large loss of raw materials and work man-hours.
In addition, if the matrix resin uses a thermoplastic resin having a melting point 20 ° C. lower than the melting point or softening point of the reinforcing fiber, a temperature close to the melting temperature Tm of the matrix resin is applied as preheating of the reinforcing fiber bundle. There is no problem. The appropriate surface temperature (preheating) of the reinforcing fiber bundle varies depending on the reinforcing fiber and matrix resin used, but the surface temperature of the reinforcing fiber bundle is relative to the temperature Tm of the matrix resin in the resin pool in the crosshead. From the viewpoint of physical properties and continuous stable productivity of the obtained long fiber reinforced thermoplastic resin linear material, Tm + 0 ° C. to Tm−50 ° C. is particularly preferable.

<Relationship between the extrusion nozzle hole diameter in the extrusion coating step and the hole diameter at the tip opening of the sheath core>
In the extrusion coating step (2) of the production method of the present invention, the discharge hole portion A of the extrusion nozzle 23 shown in FIG. 8 has a land L of 2 mm or more, and when the hole diameter is A, toward the discharge side, The upper bottom of the extrusion nozzle is cut out in a truncated cone shape, and the angle θ at which the truncated cone inclined line 232 and the discharge hole wall surface line 231 cross each other in the thickness direction cross section of the extrusion nozzle 23 exceeds 90 °. The hole diameter B of the opening at the tip of the sheath core is 105 to 360% larger than the discharge section hole diameter A. The crosshead die 2 having the sheath core 21 is extruded and coated with molten thermoplastic resin. Is done.
Referring to FIG. 8, if the land L of the extrusion nozzle 23 is 2 mm or more, a high pressure is applied to the portion of the extrusion nozzle 23, which makes it difficult to form voids in the linear object (product), and the molten thermoplastic resin This is preferable in that it easily flows into the molten resin contact portion 203 of the guide core metal in the die and the outer diameter of the linear object can be easily controlled. Moreover, if the angle θ exceeds 90 °, it is preferable in that the flow direction of the matrix resin in the traveling direction and the backward traveling direction of the reinforcing fibers F can be controlled.
The diameter B of the opening at the tip of the sheath core 21 is 105 to 360% in terms of the diameter ratio (B / A) in relation to the diameter A of the extrusion nozzle. When the B / A is 105% or more, the matrix resin can easily flow into the molten resin contact portion 203 of the guide core in the die, and by 360% or less, the amount of the molten thermoplastic resin flowing through the guide core is This is preferable in that the amount of molten thermoplastic resin discharged from the extrusion nozzle can be balanced.

<Guide guide for guide mandrel>
In the long fiber reinforced thermoplastic resin linear material of the present invention, the convergence guide preferably satisfies the following requirements (a) or two requirements (a) and (b).
(A) The hole diameter Dc of the central portion through hole of the convergence guide is 50 to 100% with respect to the outer diameter Dp of the long fiber reinforced thermoplastic resin linear material.
(B) The fan-shaped lower side diameter Dfc is twice the sector-shaped lower side radius forming the radial fan-shaped through hole of the convergence guide, and the sector-shaped lower side diameter Dfc is 105-105 with respect to the outer diameter Dp of the long fiber reinforced thermoplastic resin wire. 360%.
First, as shown in FIG. 5 and FIG. 6C, the requirement (a) is that the central through hole 202Ca or 202Cb of the converging guide of the guide mandrel 20 is disposed inside the linear object. From the viewpoint of arranging the reinforcing fiber bundle inside the linear object, the outer diameter of the long fiber reinforced thermoplastic resin linear object to obtain the hole diameter Dc is a hole through which the fiber bundle is inserted. It is preferable to make it 50 to 100% of Dp, and if it is this range, the reinforcing fiber bundle converged by the central portion through holes 202Ca and 202Cb is not exposed on the surface, and the reinforcing effect of the linear object is obtained. It can be expressed.
On the other hand, the requirement (b) is that the radial fan-shaped through holes 208b are formed according to the number of reinforcing fiber bundles to be exposed on the surface of the linear object as shown in FIGS. 6 (B) and 6 (C). The fan-shaped upper side diameter Dfc is twice the sector-shaped upper side radius of the radial fan-shaped through hole 208b, and the sector-shaped upper side diameter Dfc is 105 to 360% with respect to the outer diameter Dp of the long fiber reinforced thermoplastic resin wire. In this range, a predetermined number of reinforcing fiber bundles can be exposed on the outer periphery of the linear object.
Further, the upper side of the radial fan-shaped through hole 208b has a concentric curvature with respect to the center of the central through hole, and the required number of reinforcing fibers to be exposed by the tension applied to the reinforcing fiber bundle or the like. The bundle moves to substantially the middle part of the fan-shaped upper side, and can be arranged almost evenly on the outer periphery of the linear object.

  In the manufacturing method of the present invention, the reinforcing fiber bundles F drawn from the creel 1 guide the reinforcing fiber bundles F to the predetermined central through holes 202C of the convergence guide ( Before the insertion), the separation guides 201a and 201b shown in FIGS. 5A and 6A are inserted into predetermined holes. The reinforcing fiber bundle to be exposed is guided (inserted) into the hole arranged on the outermost periphery of the separation guide 201b in FIG.

In this invention, it can be set as the linear thing formed by exposing the required number of reinforcing fiber bundles on the surface.
That is, in a long fiber reinforced thermoplastic resin linear material composed of a matrix resin which is a thermoplastic resin and a long fiber reinforcing fiber bundle, the reinforcing fiber bundle is impregnated with the matrix resin in a cross section perpendicular to the longitudinal direction. The fiber bundle has a non-impregnated portion, and some of the fibers of the reinforcing fiber bundle are exposed on the surface of the linear object, for example, at 6 to 12 separate positions, respectively. It can be set as the continuous fiber reinforced thermoplastic resin linear thing formed continuously in a longitudinal direction.
The long fiber reinforced thermoplasticity for vehicle seats is such that the length l of each fiber exposed portion of the reinforcing fiber bundle exposed on the surface in the cross section of the linear object is in the range of 0.3 mm to 0.7 mm. In the case of using a resin linear material, it is preferable.
By exposing the reinforcing fiber bundle to the surface of the required number of linear objects, for example, when used as a member for attaching a skin material such as a cushion of a chair, the long fibers of the exposed part of the linear object when insert-molded The single fiber of the reinforcing fiber bundle and the foaming agent are anchored to each other, so that the function as a chair member can be expressed.

In particular, in the case of a long fiber reinforced thermoplastic resin linear material for vehicle seats, the length of the outer circumference calculated from the assumed outer diameter of the linear material with respect to the total length of the exposed fiber portions in the cross section of the linear material It is more preferable that the fiber exposure rate calculated as the ratio is 20 to 60%.
The exposure rate of the fiber is appropriately determined in accordance with the physical properties of the molded product after the insert molding, which is required for the use of the linear product, for both the number of exposed fibers and the exposure rate.

(Calculation of the number of exposed fibers and the fiber exposure rate of the long fiber reinforced thermoplastic resin linear material)
In the method for producing a long fiber reinforced thermoplastic resin linear product of the present invention, the number of exposed fiber portions and the exposed fiber rate are determined by the following procedure.
(I) A long-fiber reinforced thermoplastic resin linear material is cut into a length of about 1 cm in a direction orthogonal to the longitudinal direction, and a digital microscope (manufactured by KEYENCE, product name: VHX-5000) is so cut. ) Is fixed on the table with clay.
(Ii) The sample is observed with reflected light at a magnification of 30 times, and the number of fiber bundles exposed on the surface of the long fiber reinforced thermoplastic resin linear material is counted. (= Number of exposed fibers)
(iii) Using the distance calculation function built in the digital microscope, the length of the exposed fiber portion (the portion not covered with the matrix resin) on the surface is calculated one by one. (= Fiber exposed length at one location)
(Iv) The total fiber exposed portion length is obtained, and the fiber exposure rate is calculated by the following formula from the circumferential length of the long fiber reinforced thermoplastic resin linear material obtained from the outer diameter.
Fiber exposure rate (%) = [(total length of exposed fiber) / (circumferential length)] × 100
The circumferential length of the long fiber reinforced thermoplastic resin linear material is calculated from the assumed outer diameter of the long fiber reinforced thermoplastic resin linear material. In the observation of (ii) above, the assumed outer diameter is calculated by calculating the average from the maximum diameter and the minimum diameter of the portion having the matrix resin (thermoplastic resin) of the long fiber reinforced thermoplastic resin linear material as the outer surface. The outside diameter Da is not seen.

The reinforcing fiber bundle used in the method for producing the long fiber reinforced thermoplastic resin linear material of the present invention will be described below.
(Reinforcing fiber bundle)
The reinforcing fibers (bundles) used in the production of the fiber-reinforced thermoplastic resin linear material of the present invention are not particularly limited, but include inorganic fibers having no melting point such as glass fibers and carbon fibers, and various thermoplastic resins. A long fiber (filament) -like reinforcing fiber.
As a reinforcing fiber bundle made of thermoplastic resin, one or a plurality of types selected from polyethylene terephthalate fiber, polybutylene terephthalate fiber, polynaphthylene phthalate fiber, polytremethylene terephthalate fiber, polyacrylonitrile fiber, and aliphatic polyamide fiber are used. Alternatively, mixed fibers can be advantageously selected.
As described above, the melting point (Tfm) of the thermoplastic resin fiber needs to be higher than the melting point (Tmx) of the matrix resin. If it is low, the fibers may melt and break inside the extrusion die. These melting point differences Tfm−Tmx are preferably approximately 20 ° C. or more.

The matrix resin that is the thermoplastic resin used in the present invention is not particularly limited, but is selected from thermoplastic resins having a melting point lower than the melting point or softening point of the thermoplastic fiber used for the reinforcing fiber bundle. More specifically, polyolefins such as polypropylene, polyethylene and polybutylene, and polyesters such as polyethylene terephthalate (PET), polybutylene terephthalate (PBT), polytrimethylene terephthalate (PTT), polyethylene naphthalate (PENp), and liquid crystal polyester. Resins, polystyrene (PS), acrylonitrile-butadiene-styrene ABS), styrene-based resins such as acrylonitrile-acrylic-styrene (AAS), acrylonitrile / ethylene propylene rubber / styrene (AES), urethane resin, polyoxymethylene (POM) , Polyamide (PA), polycarbonate (PC), polymethyl methacrylate (PMMA), polyvinyl chloride (PVC), polyphenylene sulfide (PPS), Rephenylene ether (PPE), modified PPE, polyimide (PI), polyamideimide (PAI), polyetherimide (PEI), polysulfone (PSU), modified PSU, polyethersulfone (PES), polyketone (PK), polyether Examples include ketone (PEK), polyether ether ketone (PEEK), polyether ketone ketone (PEKK), polyarylate (PAR), polyether nitrile (PEN), phenolic resin, and phenoxy resin. The thermoplastic resin as the matrix resin may be a copolymer or modified body of the above resin and / or a resin blended with two or more kinds.
Among these, from the viewpoint of moldability and lightness, a polyolefin resin having a melting point lower by 20 ° C. or more than the melting point or softening point of the reinforcing fiber is preferable, and for example, a polypropylene resin is particularly preferable.

The matrix resin, which is a thermoplastic resin used in the present invention, has a melt flow rate (MFR) (230 ° C., 21.18 N load) of 20 to 100 g / 10 min from the viewpoint of impregnation into the reinforcing fiber bundle. It is preferable that it is the range of these.
If the MFR is 20 g / 10 min or more, the reinforcing fiber bundles can be impregnated, and the reinforcing fiber bundles are less likely to be bundled together, and the reinforcing effect by the reinforcing fiber bundle is exhibited. In addition, when the MFR is 100 g / 10 min or less, the physical properties of the resin are not significantly lowered, and the FRTP linear material is not easily broken during bending.
The thermoplastic resin used as the matrix resin includes, as necessary, an inorganic filler such as talc, a flame retardant, a conductivity imparting agent, an ultraviolet absorber, an antioxidant, a thermal stabilizer, an antistatic agent, a colorant, You may mix | blend a pigment, dye, etc.

<Cross sectional shape etc. of long fiber reinforced thermoplastic resin wire>
The cross-sectional shape of the linear object obtained by the manufacturing method of the present invention is not limited to a perfect circle, and can take various shapes such as an ellipse and a shape with irregularities.
In addition, the cross-sectional shape of the fiber bundle in the cross-section of the linear object is not limited to a perfect circle, and may be an ellipse or a polygon.
Furthermore, the distribution of reinforcing fiber bundles (islands) in the cross-section of the linear object is not necessarily uniform, but it is preferable that the distribution is point-symmetrical with respect to the center of the cross-section of the linear object. If the fiber bundle distribution in the cross section is extremely biased, the ease of bending changes depending on the direction in which the linear object is bent, and not only is it difficult to handle, but there is a possibility that the fiber bundle may be easily broken in a specific direction.
Further, the islands formed by the reinforcing fiber bundle are not necessarily clearly separated by the matrix resin, and the neighboring may be partially in contact with each other.
The number of reinforcing fiber bundles (islands) needs to be 3 or more and 50 or less. If it is less than this, it will be easy to bend at the time of bending, and if it is more than this, the heat formability will be lowered.
The size of the reinforcing fiber bundle (island) is not necessarily uniform, and the maximum island area may be about five times the minimum island area. That is, the reinforcing fiber bundles having different fineness and the reinforcing fiber bundles having different types may be used.

  EXAMPLES Hereinafter, although an Example demonstrates this invention, this invention is not limited to these Examples at all.

Example 1
(Preliminary withdrawal process)
As the reinforcing fiber bundle F, 25 polyethylene terephthalate multifilaments (manufactured by Toray, monofilament fineness 11.6 dtex) of 1670 dtex / 144 f are drawn out from the creel 1, passed through an unheated preheating device, and shown in FIG. One of the separation guides 201a having 25 holes with a diameter of 1 mm in one metal plate is passed through one hole, and then all 25 fibers are passed through the circular metal plate with one hole with a diameter of 2.5 mm. The reinforcing fiber bundle is passed through the converging guide 202Ca opened at the center of the individual piece, and the reinforcing fiber bundle is not included in the converging guide 202a so that the longitudinal cross section becomes a sea-island type linear object without the reinforcing fiber bundle exposed on the surface of the linear object. Arranged.
Next, the separation guide 201a and the convergence guide 202a that are passed through the reinforcing fiber bundle F shown in FIG. 7 are fitted into the grooves 204 and 205 of one half of the half-shaped guide mandrel 20 for mounting inside the crosshead die, A circular extrusion nozzle having a diameter of 3.2 mm, in which the reinforcing fiber bundle group passed through the convergence guide 202a is attached to the tip of the die by overlapping with the other half-divided guide core bar to form a cylindrical guide core bar 20. Then, a guide mandrel (guide holder) 20 was attached to the back of the crosshead die body 2.

(Drawing tension of reinforcing fiber bundle)
The multi-fragment, which is a reinforcing fiber bundle, is attached to a feeding stand in a state of being wound around a paper tube, and pulled out via a loading type tensor TC1 as tension adjusting means TC shown in FIG. By this tension adjusting means TC1, the tension (tension) of each reinforcing fiber bundle was adjusted to 20 g / line.

(Manufacture of long fiber reinforced thermoplastic resin wire)
The temperature of the preheating device PH is raised to 200 ° C. while taking the reinforcing fiber bundle group that has passed through the extrusion nozzle 23 through the cooling water tank 3 and using the belt type take-up device 4 at a speed of 3 m / min. The melt extruder was started and melted at an extrusion temperature of 220 ° C., and then a polypropylene resin (manufactured by Prime Polymer, MFR: 55 g / 10 min: 230 ° C., 21.18 N with talc, copper damage inhibitor, blue for rigidity adjustment) The master batch for attaching was blended, and the actual MFR was 34.2 g / 10 min). In addition, the discharge hole portion of the extrusion nozzle has a land L of 4 mm, a hole diameter A of 3.2 mm, and is cut out in a truncated cone shape with an upper base A of 3.2 mm toward the discharge side. In the cross section of the extrusion nozzle 23 in the thickness direction, the angle θ at which the frustoconical inclined line 232 and the line 231 of the discharge hole wall face 231 is 125 °, and the hole diameter B of the opening of the opposite sheath core is 6.4 mm. The crosshead die 2 having a sheath core having a relationship of 200% larger than the discharge portion hole diameter A was used. The molten polypropylene resin enters from the outer periphery of the sheath core 21 and reaches the tip of the sheath core 21, and then a part is discharged in the direction of the extrusion nozzle together with the fiber bundle passing through the sheath core. The fiber 21 flows backward from the tip of the core 21 toward the opening of the sheath core, and impregnates a part of the reinforcing fiber bundle F that has passed through the guide core metal 20 while staying there. Finally, the shape is given by the extrusion nozzle 23. This was taken out while being cooled in the cooling water tank 3 to obtain a long fiber reinforced thermoplastic resin wire (rod) having a diameter of 3.4 mm. A schematic diagram of a cross section of the obtained long fiber reinforced thermoplastic resin is shown in FIG. It shows in Table 1 about the physical property etc. of the obtained linear thing.

Example 2
(Preliminary withdrawal process)
As a reinforcing fiber bundle, 25 1100 dtex / 95 f polyethylene terephthalate fibers (manufactured by Toray) were passed through a tensor as a tension adjusting means TC and an unheated preheater PH from a creel, and 25 mm of a diameter of 1 mm on a circular metal plate. One of the holes in the separation guide 201b (FIG. 6 (A)) with a plurality of holes, one through each, and then the outer six holes arranged at a position of 18 mm PCD among the holes in the separation guide 6 of the converging guide 202b in which one hole having a diameter of 2.0 mm is formed at the center of the circular metal plate shown in FIG. 6B and six radial fan-shaped holes are formed around it. The remaining 19 fibers passed through 19 holes inside the separation guide, one by one through the 6 fan-shaped holes, were passed through the central hole 202Cb. When the fibers outside the separation guide are passed through the fan-shaped holes 208b of the convergence guide 202b, the fibers are linearly passed so that the fibers do not intersect each other. In addition, the convergence guide whose diameter Dfc of the fan-shaped lower side 2021 of a radial fan-shaped hole is 7.0 m was used.
Next, in order to attach the separation guide 201b and the convergence guide 202b to the inside of the same crosshead die 2 as in the first embodiment, the separation guide 201b and the convergence guide 202b are fitted in the grooves 204 and 205 of one half-shaped guide core bar 20 and the other half-section is opposed. A cylindrical guide core 20 is formed by superimposing it with a cylindrical guide core, and the reinforcing fiber bundle group passed through the convergence guide 202b is passed through a circular extrusion nozzle 23 having a diameter of 3.2 mm attached to the tip of the die. The guide mandrel 20 was attached to the back of the crosshead die body 2. At this time, the outer six fiber bundles conducted to the position of PCD φ18 mm among the holes of the separation guide were in contact with the inner wall of the discharge hole of the extrusion nozzle 23.
Note that the discharge hole portion of the extrusion nozzle has a land L of 4 mm, a hole diameter A of 3.2 mm, and is hollowed out into a truncated cone shape having an upper base of 3.2 mm toward the discharge side. In the cross section in the thickness direction of the die, the angle θ at which the frustoconical inclined line 232 and the discharge hole wall surface line 231 intersect is 125 °, the hole diameter B at the tip of the opposite sheath core is 6.4 mm, and the discharge hole diameter A die having the same sheath core as in Example 1, which is 200% larger than A, was used.

(Molding of long fiber reinforced thermoplastic resin wire)
The reinforcing fiber bundle group passed through the extrusion nozzle 23 is passed through the cooling water tank 3 and then taken up at a speed of 5 m / min using the belt-type take-up device 4. Tension measurement by adjusting the load by passing the reinforcing fiber bundle F through the tensor TC1 with two disc-shaped ceramic plates inserted in the central axis J as tension adjusting means, and placing the weight W on the disc. A device (Yokogawa Electronics Co., Ltd., tension meter T-101) is used to adjust the tension to 10 g / piece, and it is divided into upper and lower halves and forms a cylindrical shape when assembled. With the preheating device PH equipped with Technology, Leister Electron), the surface temperature of the reinforcing fiber bundle is set to 200 ° C., which is 20 ° C. lower than the extrusion temperature 220 ° C., and the melt extruder E is started. After melting at an outlet temperature of 220 ° C., a polypropylene resin (manufactured by Prime Polymer, MFR: 55 g / 10 min: 230 ° C., 21.18 N), as shown in FIG. 9 (C), inside the die (221 to 223) and the guide core 20 molten resin contact portions 203 were supplied. The long fiber reinforced thermoplastic resin linear product 101 having a diameter of 3.4 mm is taken out while being cooled in the cooling water tank 3 filled with cooling water. Obtained. A schematic diagram of a cross section of the obtained long fiber reinforced thermoplastic resin linear product 101 is shown in FIG.

  The number of exposed fiber portions of the long fiber reinforced thermoplastic resin filament obtained in Example 2 was 6. The fiber exposure rate was 28%. The pulling strength was 18.3 N, and a high result was obtained as compared with the long fiber reinforced thermoplastic resin linear material having no fiber exposure or little exposure. These results are summarized in Table 1.

Examples 3-7, Comparative Examples 1-3
In order to establish the mass production technology for long-length long fiber-reinforced thermoplastic resin filaments, the production rate is 20 m, especially for long-fiber-reinforced thermoplastic resin filaments with a predetermined number of reinforcing fiber bundles exposed on the surface. As / min, the stable continuous productivity and the appearance of the exposed fiber bundle were evaluated.
In the production conditions of Example 2, an example in which the pulling tension of the reinforcing fiber bundle from the creel was 3 g / line to 120 g / line, and the preheating temperature of the reinforcing fiber bundle was normal temperature (20 ° C.) to 200 ° C., comparative example The stability (continuous) productivity and the degree of fiber exposure were observed and evaluated as follows.
(I) Continuous productivity: The production length of 5000 m was evaluated as follows based on the number of fiber breakage of reinforcing fibers during the production time, assuming that the production length was about 4 hours at a production rate of 20 m / min. .
○: No fiber breakage during 4 hours, Δ: One fiber breakage during 4 hours, X: Two or more fiber breaks (ii) Fiber exposure: Six reinforcements on the outer peripheral surface of the linear object as in Example 2. In the case of arranging the fiber bundles for exposure, the degree of fiber exposure was evaluated.
○: 1/3 or more of the reinforcing fiber bundle is exposed (good), Δ: 1/3 or less exposed or unstable, ×: fiber bundle is not exposed.
The results are summarized in Table 2.

From Table 2, in Comparative Example 1 in which the pulling tension from the creel is 3 g and the preheating temperature is 200 ° C., the fiber bundle for reinforcement is broken three times during the four continuous productivity times, and the exposed state of the fiber is “ Δ ”. In Comparative Example 2, thread breakage occurred four times as in Comparative Example 1 with a drawing tension of 5 g / bar and a preheating temperature of room temperature (20 ° C.), but the degree of fiber exposure was good. When the drawing tension was 5 g / bar and the preheating temperatures were 150 ° C. (Example 3) and 200 ° C. (Example 4), one thread breakage was observed during production for 4 hours in Example 3, but exposure was not possible. Both degrees were good. The preheating temperature is 200 ° C., and the pulling tension is 5 g / line (Example 4), 10 g / line (Example 5 = Example 2), 50 g / line (Example 6), 100 g / line (Example 7), In the case of 120 g / line (Comparative Example 3), when the pulling tension exceeded 50 g / line, the degree of fiber exposure tended to deteriorate, and in Examples 6 and 7, it was “Δ”. As for continuous productivity, one thread breakage occurred in Example 7 (“Δ”), and in Comparative Example 3, both continuous productivity and fiber exposure degree were “x”.
It was confirmed that even if the production speed was greatly improved by Examples 3 to 7, stable production was possible and the degree of exposure of the reinforcing fiber bundle was good.

The method for producing a long fiber reinforced thermoplastic resin filament according to the present invention is performed by adjusting the degree of impregnation of the matrix resin, which is a thermoplastic resin, into the long fiber reinforcing fiber bundle and the degree of exposure of the surface exposed fiber bundle. It is possible to provide a method that enables continuous production of long fiber reinforced thermoplastic resin filaments with excellent physical properties (reproducibility) in a stable and reproducible manner. It can be used as a method for producing a non-metallic member that can be used in place of a use that has been used.
Further, a reinforcing fiber bundle that can be used as a long fiber reinforced thermoplastic resin linear material for vehicle seats has an unimpregnated portion that is not impregnated with the matrix resin in a cross section perpendicular to the longitudinal direction. Each of the fiber bundles is partly exposed in the form of a separate bundle on the surface of the long fiber reinforced thermoplastic resin wire, and is continuous in the longitudinal direction. The fiber bundle for reinforcement is not impregnated with the matrix resin. Long fiber reinforced thermoplastic resin linear shape that can exhibit the bond between the long fiber reinforced thermoplastic resin linear material and the foam by impregnating with soft polyurethane foam resin, which is the cushion material of the seat, at the time of seat pad molding It can be used as a production method for stably producing products continuously.

DESCRIPTION OF SYMBOLS 1 Creel 2 Melt extruder Crosshead die part 3 Water cooling tank 4 Take-out apparatus 20 Guide core 21 Saya core 22 Crosshead die main body 23 Extrusion nozzle 231 Discharge hole part wall line 232 Frustum inclined line 100 Long fiber reinforced thermoplastic resin line Form (first aspect)
101 Linear fiber reinforced thermoplastic resin (second aspect: required number surface exposed type)
201a, b Separation guide 202a, b Convergence guide 202C Convergence guide central through hole 2021 Fan-shaped lower side 203 Molten resin impregnated portion 203S Impregnation start point 203E in molten resin impregnated portion 204E Impregnation end point 204, 205 Guide retaining groove 206 Flange 207 Mounting hole 208 Radial fanned portion or through hole guide portion 209 of the converging guide Resin inflow hole 221 In-die resin flow path 222 In-die inclined portion resin flow path 223 Impregnation section resin flow path A Extrusion nozzle hole diameter B Saya core tip opening Diameter D disk E melt extruder F long fiber reinforcing fiber bundle Fo 'exposed reinforcing fiber Fi' internal reinforcing fiber G1, G2 first and second guides (thread guide)
G3 Collective guide GB Guide bar L Extrusion nozzle land l Fiber exposed part length M Matrix resin S Sea I Island TC Tension adjusting means PH Preheating device W Weight Rfc Fan-shaped lower radius of convergence guide Rc Convergence guide central hole radius Dfc Convergence Guide fan bottom diameter Dc Convergence guide center through hole diameter

Claims (8)

A method for producing a long fiber reinforced thermoplastic resin linear product comprising a matrix resin which is a thermoplastic resin and a fiber bundle for reinforcing long fibers,
(1) A long-fiber reinforcing fiber bundle having a predetermined number of twists is drawn from a required number of creels through a tension adjusting means, and is passed through an unheated preheating device, and includes a separation guide, a molten resin impregnation portion, and a convergence guide. The fiber bundles are sequentially arranged and inserted through the predetermined through holes of the separation guide and the convergence guide of the guide core, the guide core is attached to the crosshead die main body, and then provided with a sheath core and an extrusion nozzle. A preliminary drawing step of a bundle of long fiber reinforcing fiber bundles, which is led to a die, a cooling tank, and a drawing device;
(2) While driving the take-up device and taking up the group of long fiber reinforcing fiber bundles at a predetermined speed, a tension of 5 to 100 g is applied to the reinforcing fiber bundle via the tension adjusting means. And driving the melt extruder while heating the reinforcing fiber bundle by heating the preheating device, supplying the thermoplastic resin to the crosshead die, and impregnating the guide core metal with the molten resin Each separated reinforcing fiber bundle is brought into contact with the molten thermoplastic resin in the part and die, and each reinforcing fiber bundle is partially impregnated with the thermoplastic resin, followed by a convergence guide, and a predetermined cross-sectional shape. A step of extruding and coating the long fiber reinforcing fiber bundle group as a linear object under pressure with a die having an extrusion nozzle of
(3) a step of cooling and solidifying the extrusion-coated linear material and taking it out;
Have
In the step of extrusion coating the linear material, the heating of the reinforcing fiber bundle in the preheating device is such that the surface temperature of the reinforcing fiber bundle is Tm to Tm-200 with respect to the temperature Tm of the molten thermoplastic resin. A method for producing a long fiber reinforced thermoplastic resin linear product, characterized in that the temperature reaches a range that reaches ° C.   In the (2) extrusion coating step, the discharge hole portion of the extrusion nozzle 23 has a land L of 2 mm or more, and when the hole diameter of the discharge hole portion is A, the extrusion nozzle has an upper bottom A toward the discharge side. The angle θ between the frustoconical inclined line 232 and the nozzle discharge hole wall surface line 231 exceeds 90 ° in the cross section in the thickness direction of the extrusion nozzle 23, and the opposing sheath cores 21 are opposed to each other. 2. The length according to claim 1, wherein the molten thermoplastic resin is extrusion-coated by a die having a sheath core having a relationship in which the hole diameter B of the opening at the tip is 105 to 360% larger than the discharge part hole diameter A. A method for producing a fiber-reinforced thermoplastic resin wire. The method for producing a long fiber-reinforced thermoplastic resin wire according to claim 1 or 2, wherein the convergent guide of the guide core metal satisfies the following requirements (a) or two requirements (a) and (b). .
(A) The hole diameter Dc of the central portion through hole of the convergence guide is 50 to 100% with respect to the outer diameter Dp of the long fiber reinforced thermoplastic resin linear material.
(B) The fan-shaped lower side diameter Dfc is twice the fan-shaped upper side radius forming the radial fan-shaped through hole of the convergence guide, and the sector-shaped lower side diameter Dfc is 105 to 105 relative to the outer diameter Dp of the long fiber reinforced thermoplastic resin wire. 360%.   The method for producing a long-fiber-reinforced thermoplastic resin linear product according to any one of claims 1 to 3, wherein a necessary number of reinforcing fiber bundles are exposed on the surface of the linear product.   The reinforcing fiber bundle is a multifilament in which fibers having a single fiber fineness of 1.5 to 30 dtex are bundled by 80 to 150 f and have a twist of 2 to 500 times / m. The manufacturing method of the long fiber reinforced thermoplastic resin linear material of Claim 1.   The reinforcing fiber constituting the reinforcing fiber bundle is made of a thermoplastic resin, and the matrix resin is a thermoplastic resin having a melting point that is lower by 20 ° C or more than the melting point or softening point of the reinforcing fiber. 6. The method for producing a long fiber reinforced thermoplastic resin linear product according to any one of 5 above.   The reinforcing fiber made of the thermoplastic resin is one or more kinds selected from polyethylene terephthalate fiber, polybutylene terephthalate fiber, polyethylene naphthalate fiber, polytrimethylene terephthalate fiber, polyacrylonitrile fiber, and aliphatic polyamide fiber. The manufacturing method of the long fiber reinforced thermoplastic resin linear material of Claim 6 which is a fiber.   The thermoplastic resin which comprises the said matrix resin consists of a polypropylene resin whose melt flow rate (230 degreeC, 21.18N) is 20-100 g / 10min, The length of any one of Claims 1-7 A method for producing a fiber-reinforced thermoplastic resin wire.