JP3257188B2 - Manufacturing equipment for long fiber reinforced thermoplastic resin composites - Google Patents

Description

DETAILED DESCRIPTION OF THE INVENTION

[0001]

The present invention relates to a apparatus for manufacturing continuous fiber-reinforced thermoplastic resin composite, the opening impregnation vessel (impregnation die
The present invention relates to an apparatus capable of uniformly distributing the molten resin in a horizontal direction (in the present invention, "up, down, left, right, and vertical and horizontal" are expressions for convenience of explanation).

[0002]

2. Description of the Related Art In a conventional apparatus for producing a long fiber reinforced thermoplastic resin composite, a molten resin supplied from an extruder is used.
A connecting pipe having a circular cross section connected by a flange or the like is used as a means for feeding the fiber to the opening and impregnating tank . Although this feeding method is easy, it leaves a strong tendency that the molten resin introduced into the opening and impregnating tank tends to be biased in a range close to the shape of the feeding pipe.

[0003]

In the conventional method using the above connecting pipe, it is difficult to avoid the following various situations from remaining. -The bundle of reinforcing long fibers to be opened by joining with the molten resin in the opening impregnation tank is not sufficiently opened. Therefore, the resulting complex does not exhibit the desired properties.・ As a result of the localization of the molten resin in the blind spot which often remains in the opening and impregnating tank , the resin is deteriorated, resulting in deterioration of the performance of the product, contamination of the product with foreign substances or appearance of the product (coloring Etc.) The occurrence of defects and other extraordinary products occurs.・Fiber breakage due to uneven flow in the opening impregnation tank,
Clogging of the drawing nozzle due to broken fibers , resulting in inevitable operation shutdown, etc.

[0004]

Means for Solving the Problems The present inventors have made intensive studies to solve the following problems associated with the conventional manufacturing apparatus, and as a result, have completed the present invention: 1) Opening the apparatus downstream of the extruder in the apparatus fiber impregnation vessel is connected, a resin passage inlet sectional area thereof in the connected T die between the upstream side of the downstream side and the opening impregnation vessel of the extruder
For producing long fiber reinforced thermoplastic resin composites having a large outlet cross-sectional area.

[0005] 2) A resin outlet from the T-die , the lower side of which is substantially coincident with and connected to the lower side of the resin passage inlet located at substantially the same height as the upper surface of the bottom plate of the spread impregnation tank downstream thereof. An apparatus for producing the long fiber reinforced thermoplastic resin composite according to the above.

3) The long-fiber-reinforced thermoplastic resin composite according to item 1 or 2, wherein the cross-sectional shape of the resin outlet from the T-die has at least one of an upper side curved downward and a lower side curved upward. manufacturing device. 4) The decreasing gradient Gv of the resin path in the T-die is 0.01 to 0.1.
4. The apparatus for producing a long fiber-reinforced thermoplastic resin composite according to any one of the above items 1 to 3. 5) The widening gradient Gw of the resin passage in the T-die is from 0.1 to 0.3.
Item 5. An apparatus for producing a long fiber-reinforced thermoplastic resin composite according to any one of Items 1 to 4, above. 6) The long fiber reinforced thermoplastic resin composite according to any one of the above items 1 to 5, wherein the degree of curvature Rc of at least one of the upper side and the shorter side at the exit of the resin passage in the T-die is 0.01 to 0.05. Manufacturing equipment. 7) An apparatus in which an open fiber impregnation tank is connected downstream of the extruder
Between the downstream end of the extruder and the upstream end of the opening impregnation tank
The resin passage in the T-die connected to the
Also has a large exit cross-section, and the resin
Is 0.01 to 0.1, and the T die
Before the widening gradient Gw of the resin passage inside is 0.1 to 0.3.
7. The long fiber reinforced thermoplastic resin composite according to any one of items 1 to 6 above.
Coupling manufacturing equipment.

[0007]

BEST MODE FOR CARRYING OUT THE INVENTION [Description Based on Drawings] The apparatus of the present invention will be specifically described below with reference to the drawings. However, the present invention is not limited to this (note that a drawing substitute photograph showing the effect of the present invention is arranged in FIG. 3A and FIG. 3B).

FIG. 1A is a schematic process diagram showing a conventional manufacturing apparatus and a manufacturing apparatus of the present invention in comparison. Parts common to both devices are denoted by the same reference numerals. FIG. 1A is a schematic process diagram of a conventional manufacturing apparatus. In FIG. 1A, reference numeral 1 denotes an extruder, and a flow of molten resin flows through a connecting pipe 2 via a connecting pipe 2 connected to a downstream end thereof.
Is supplied to an open fiber impregnation tank (impregnation die) 3 connected to the downstream end of the fiber . A long fiber roving (bundling body) 4 for reinforcement is separately supplied from the raw material 41 to the open fiber impregnation tank 3, merges with the molten resin flow in the open fiber impregnation tank 3, and enters the open fiber impregnation tank 3. The installed fiber-spreading pin members 31a, 31b, 31c and 3
Passing through a staggered path formed by them while abutting on 1d. As the roving 4 passes through the staggered path, the roving 4 is opened by the resin flow, and the molten resin is impregnated as much as possible between the monofilaments and / or the low bundles formed by opening the long rovings. A reinforced thermoplastic resin composite 5 is obtained.

FIG. 1B is a schematic process diagram of the manufacturing apparatus of the present invention. In FIG. 1B, the extruder 1 and the fiber opening are performed.
A T-die 22 is installed between the impregnation tank 3 and the impregnation tank 3. In other respects, it is essentially the same as the conventional manufacturing apparatus in FIG. The role of the T-die 22 shown in FIG. 1 (b) is that the molten resin flow supplied from the extruder 1 via the connecting pipe 21 is previously fed in the lateral direction (in the horizontal plane, perpendicular to the molding direction). Spread impregnating tank 3 in a state of being uniformly distributed (developed)
To supply to

FIG. 2 shows the detailed shape and structure of the T-die 22 which is the main feature of the manufacturing apparatus of the present invention. In FIG. 2A, the T-die 22 is located between the upstream end wall 22a and the downstream end wall 22b. In this structure, a top plate 22ct and a bottom plate 22cb are provided between the two with a resin passage 22s therebetween. It is important that at least the top plate 22ct be installed in the vertical cross-sectional shape of the resin passage 22s in such a manner that the height thereof is reduced toward the opening and impregnating tank 3 as shown in FIG. . Normally, the lower surface of the top plate 22ct and the upper surface of the bottom plate 22cb both reduce the height of the resin passage 22s with substantially the same gradient (absolute value).

The taper gradient Gv in the vertical cross section of the resin passage 22s is expressed by the following equation (assuming that the vertical cross section of the resin passage 22s is substantially symmetric with respect to the center line). A decreasing gradient of the resin passage: Gv = (hi1-he1) /
(2 × L) [hi1: height of resin passage entrance; he1: height of resin passage exit; L: length of resin passage].

[0012] The main object of the manufacturing apparatus of the present invention is the T
In (a) 22, Gv is usually set to 0.01 to 0.1, preferably 0.015 to 0.08. The taper gradient Gv2 in the case where only the lower surface of the top plate 22ct forming the T-die 22 descends toward the opening and impregnating tank 3 (decreases the height of the resin passage 22) is expressed by the following equation.・ Reduction gradient of resin passage: Gv2 = (hi2-he2) /
L [hi2: height of resin passage entrance; he2: height of resin passage exit; L: length of resin passage].

In this case, if L is set to be equal to the above value, Gv2 becomes substantially twice as large as Gv1. However, if the decreasing gradient is increased twice as much as the above resin passage, the flow resistance of the resin may not be doubled but may be greatly increased. To avoid this situation, it is useful to set the resin passage length L of the T-die 22 to about twice.

FIG. 2B shows a widened (divergent) shape in a horizontal cross section of the T-die 22 which is the main feature of the manufacturing apparatus of the present invention. The upstream end inlet 22ai of the T-die 22 is usually circular and the downstream end outlet 22be is substantially rectangular, and the width (diameter of the circle) of the upstream end inlet 22ai is Wi,
Assuming that the width of the downstream end outlet 22be is We, the widening gradient Gw of the resin passage is expressed by the following equation. -Widening gradient of resin passage: Gw = (We-Wi) / (2 ×
L) [Wi: inlet width of resin passage; We: outlet width of resin passage;
L: length of resin passage].

Constituting the manufacturing apparatus of the present inventionT dieOn 22
In the above, the above Gw is usually 0.1 to 0.3, preferably
Is set to 0.15 to 0.25. FIG. 2 (c)Tda
I22 and the fixing plate 22s to which it is fitted
a. In FIG. 2C, the entrance 22 of the resin passage is shown.
ai is bored at the center of the upstream end wall 22a, and is the entrance of the resin passage.
The outlet 22be of the resin passage is shown horizontally long at the back of 22ai.
ing. Area of 22ai: Si = π [Wi (= hi) / 2]²  The shape of the inlet 22ai of the resin passage is not limited to a circle,
It can be shaped.

FIG. 2D shows a downstream end wall 22 b of the T-die 22. The outlet 22be of the resin passage 22 is a horizontally long rectangle, and its width is We and its height is he, and the area of the outlet is represented by the following equation. Area of 22be: Se = We × he In the T die 22 which is the main object of the manufacturing apparatus of the present invention, S
It is important that i <Se . As long as this condition is satisfied, at least one of the upper and lower sides of the resin passage outlet 22be is curved inward, ie, a "peg type" (also known as a "drum type").
This is also beneficial for equal distribution of the resin flow.

That is, making the shape of the resin passage outlet 22be a "thread-winding type"("hourglassshape") is useful for correcting the tendency of the resin amount to increase near the center of the resin passage. The reason is that the resistance received by the resin flow near the center of the resin passage is less than that near the side edges.

If the degree of curvature Rc can be approximated by an arc, the height he at both ends of the resin passage outlet 22be and the height hec at the center are conveniently expressed by the following equation (here, both upper and lower sides). It is assumed to be curved to the same extent). -Curvature: Rc = (he-hec) / (2 * We) In the manufacturing apparatus of the present invention, Rc is usually 0.01 to
0.05, preferably 0. A setting of 015 to 0.035 is sufficient for ordinary purposes.

In the manufacturing apparatus of the present invention, the downstream side outlet 22be of the T-die 22 is installed at a position where the lower side thereof coincides with the bottom side of the resin inlet (not shown) of the spread impregnation tank 3. That is, the resin inflow port of the fiber opening and impregnating tank 3 is usually installed at substantially the same height as the upper surface of the bottom plate 3b.

[Thermoplastic Resin] The thermoplastic resin which can be used in the present invention includes any commercially available one. For example, poly-α-olefin resin,
Examples thereof include a polyester resin, a polyamide resin (nylon), and a polycarbonate resin. Among these, poly-α-olefin resins are preferable for ordinary applications. Of course, other resins may be preferable depending on the property value required from the application. For example, in an application that needs to withstand use at a higher temperature, a polyester resin such as a polyethylene terephthalate resin (abbreviated as “PE”) is used.
T ") or polybutylene terephthalate resin (abbreviation" PBT ") or polyamide resin (alias" nylon ")
For example, 6-nylon, 7-nylon, 11-nylon, 66-nylon, 610-nylon, and 612-nylon are preferable. In applications where impact resistance is particularly required, bisphenol-based polycarbonate resins such as poly [2 , 2-butylidenebis (4-hydroxyphenyl) carbonate] is preferred.

Examples of the poly-α-olefin resin include the following: ethylene, propylene, 1-butene, 4-methyl-1
-Homocrystalline polymers of monomers selected from α-olefins (1-olefins) such as pentene, 1-hexene and 1-decene, and crystalline copolymer resins of two or more such monomers, and A composition comprising two or more. Among them, preferred from a practical point of view are crystalline polypropylene resins, propylene-ethylene copolymer crystalline resins and polyethylene resins, and compositions comprising two or more of these. At least one partially modified product selected from the above poly-α-olefin resins, for example, a modified polymer containing maleic acid or maleic anhydride as a modifier substantially in a grafted state, or the α-olefin resin An at least partially modified product of a low-crystalline polymer or an amorphous polymer of an olefin. Of these, preferred are maleic anhydride-modified polyethylene resin, maleic anhydride-modified polypropylene resin, maleic anhydride-modified ethylene-propylene copolymer resin or the copolymer elastomer or maleic anhydride-modified α-olefin. It is a thermoplastic elastomer.

[Reinforcing long fiber] The material forming the reinforcing long fiber used in the practice of the present invention can be selected from inorganic fibers and organic fibers. Examples of the inorganic fiber include glass fiber, rock wool (rock wool), asbestos, whisker (whisker), metal fiber, and carbon fiber. Examples of the organic fibers include wholly aromatic polyamide fibers and wholly aromatic polyester fibers.

These long fibers are monofilaments (single filaments).
Article) or single fiber (used not only as a form of single fiber), is often used as such form of Robin grayed was Atsumarihigashi mutually many of them present in the binder.

In the form of roving, it is difficult for each monofilament to independently exert a strengthening action, and the magnitude of the strengthening action exerted by the monofilaments is far from the expected level. Therefore, it is highly preferable that the resin be impregnated between the monofilaments in order to exert the maximum reinforcing effect. In other words, it is expected that the state in which the monofilaments of the long fibers are opened (dispersed) in the resin layer substantially parallel to the molding direction of the resin layer and independently of each other will exert the maximum reinforcing effect.

[0025]

DESCRIPTION OF THE PREFERRED EMBODIMENTS Hereinafter, a production example of a long fiber reinforced thermoplastic resin composite using the production apparatus of the present invention will be described in comparison with a production example using a conventional production apparatus. However, the present invention is not limited to this.

[0026]

Example 1 A T-die mounted on the downstream end of the extruder 1 via a connecting pipe 21 mounted on the downstream end thereof after melt-kneading while quantitatively supplying the resin mixture from the supply port of the extruder 1. 22 to feed the molten oil tree stream in the horizontal direction (horizontal
A resin inlet installed at substantially the same height as the upper surface of the bottom plate 3b of the open fiber impregnation tank 3 attached to the downstream end of the T-die 22 while uniformly dispersing in a direction substantially perpendicular to the molten resin flow in the plane. ( Not shown) and continuously supplied into the opening and impregnating tank 3.

On the other hand, the fiber impregnating and impregnating tank 3 is supplied with the glass rovings 4 from the glass roving raw material 41 while the fiber impregnating and impregnating.
The molten resin is merged with the molten resin in the tank 3, and both are joined with a pin member 31 a
31b, it was extruded a sufficiently molten resin impregnated composite into strands between each monofilament caused by opening of the glass roving through a staggered passage formed by 31c and 31d. Here, the glass roving 4 has an average fiber diameter of 17 μm and a number of filament bundles of 400.
No. 0, Tex No. 2310 for polypropylene was used.

As the T-die 22, an enlarged gradient G of a horizontal section is used.
A coat hanger type having a vertical gradient Gv0.05, a resin inlet width Wi of 8 mm, a resin inlet height he of 1 mm, and a resin passage length L of 75 mm with w0.21 was used.
The resin passage of the T-die 22 was symmetrical left and right and up and down with respect to the center line in both the horizontal cross-sectional shape and the vertical cross-sectional shape.

This is the main feature of the manufacturing apparatus of the present invention.
FIG. 3 shows a micrograph of a cross section of the long fiber reinforced composite obtained by using the T-die 22 and a micrograph of a cross section of the long fiber reinforced composite obtained by a conventional method of supplying a molten resin through a connecting pipe.

FIG. 3A is an enlarged photomicrograph of a cross section of a long fiber reinforced composite by a conventional manufacturing apparatus, and FIG. 3B is a cross sectional view of a long fiber reinforced composite by a manufacturing apparatus of the present invention. It is an enlarged microscope photograph. When both are compared, it is obvious at a glance that the fibers are distributed much more uniformly in the long fiber reinforced composite by the production apparatus of the present invention than in the composite by the conventional production apparatus.

That is, in the cross section of the composite by the conventional manufacturing apparatus [FIG. 3 (a)], the fact that the fibers are unevenly distributed in a certain area in the resin phase appears on the screen of the enlarged microscope photograph in black or gray. It can be seen from the appearance that the shadow has blurred. There is hardly any fiber present in a location away from the shaded area.
On the other hand, the cross section of the composite by the manufacturing apparatus of the present invention [FIG. 3 (b)] shows that the fibers are separated from each other and uniformly (uniformly) distributed in the resin phase. You can see from many small dots scattered on the screen. The dark black shadows are only partially visible on a small scale.

<Resin mixture> Unmodified polypropylene resin (homopolymer) [MFR (2
30 ° C; 2.16 kgf) 2 g / 10 min] Powder 9
9.20% by weight, 0.5% by weight of maleic anhydride as an unsaturated acid as a modifier, 0.1% of 1,3-bis (t-butylperoxyisopropyl) benzene as an organic peroxide
% By weight, 2,6-di-t-butyl-p as antioxidant
A mixture consisting of 0.1% by weight of cresol and 0.1% by weight of calcium stearate as a lubricant was mixed and stirred in a Henschel mixer (trade name; not shown).

The resin mixture is used as an extruder 1 as a twin screw extruder (diameter 45 mm; L / D 30; plural raw material supply ports are provided).
And the mixture was melt-kneaded (at a temperature of 200 ° C.) and extruded and granulated. The resulting modified polypropylene had an MFR (230 ° C .; 2.16 kgf) 1
It was 30 g / 10 min and the modifier graft ratio was 0.3%.

[0034]

In the manufacturing apparatus according to the present invention, the flow of the molten resin supplied from the extruder 1 via the connecting pipe 21 increases the width (horizontal length) of the inside of the T-die 22 installed at the downstream end of the pipe. The shape and the height (vertical length) reduced shape cooperate to distribute evenly in the lateral direction.

[0035]

With the apparatus of the present invention, it is possible to achieve the various effects of the following: (1) Robin grayed reinforcing long fibers to be opened merges with opening impregnation vessel with the molten resin Etc. are fully opened. Therefore, the resulting composite exhibits the desired properties. (2) Blind spots hardly occur in the opening and impregnating tank . As a result, the situation where the molten resin stays locally does not occur,
The risk of extraordinary products is almost eliminated. (3) The operation is not almost stopped due to the cause in the opening and impregnating tank .

[Brief description of the drawings]

FIG. 1A is a conceptual diagram of a conventional manufacturing apparatus, and FIG. 1B is a conceptual diagram of a manufacturing apparatus of the present invention.

FIG. 2 shows a detailed shape and structure of a T-die in the manufacturing apparatus of the present invention. FIG. 2A is a schematic longitudinal sectional view showing a state in which the T-die is connected to the opening and impregnating tank. FIG. 2B is a schematic cross-sectional view of the T-die . FIG. 2C is a schematic plan view of the upstream end wall of the T-die and a fixing plate to which it is fitted. FIG. 2D is a schematic plan view showing the downstream end wall of the T-die .

FIG. 3 (a) is an enlarged microscopic photograph (substitute drawing) showing a cross section of a composite obtained by a conventional production apparatus instead of a drawing, and FIG. 3 (b) is a production method of the present invention. It is an enlarged microscope photograph (drawing substitute photograph) which replaces a drawing and shows a section of a composite obtained by an apparatus.

[Explanation of symbols]

DESCRIPTION OF SYMBOLS 1 Extruder 2 Resin feeding connection pipe 3 Opening impregnation tank 4 Reinforcing long fiber roving 5 Long fiber reinforced thermoplastic resin composite 21 Resin feeding connection pipe 22 T die 22a T die upstream end wall 22b T Die downstream end wall 31a Opening pin member 31b Opening pin member 31c Opening pin member 31d Opening pin member 22ai T die entrance 22be T die outlet 22ct T die top plate 22cb T die bottom plate 22sa T Fixing plate for fitting the die upstream end wall LT die length he T die exit height hi T die entrance height We T die exit width Wi T die entrance width

Claims (7)

(57) [Claims] 1. An apparatus in which an opening and impregnating tank is connected to the downstream side of an extruder, wherein a resin passage in a T-die connected between a downstream end of the extruder and an upstream end of the opening and impregnating tank is provided. An apparatus for producing a long fiber reinforced thermoplastic resin composite having an outlet cross-sectional area larger than its inlet cross-sectional area. 2. A lower side of a resin outlet from the T-die is connected to and substantially coincident with a lower side of a resin passage inlet located at substantially the same height as an upper surface of a bottom plate of the opening and impregnating tank on the downstream side thereof. The manufacturing apparatus of the long fiber reinforced thermoplastic resin composite according to the above. 3. The long fiber reinforced thermoplastic resin composite according to claim 1, wherein a cross section of the resin outlet from the T-die has at least one of an upper side curved downward and a lower side curved upward. manufacturing device. 4. The reduction gradient Gv of the resin passage in the T-die is equal to 0.
The apparatus for producing a long-fiber-reinforced thermoplastic resin composite according to any one of claims 1 to 3, wherein the number is from 0.1 to 0.1. 5. A widening gradient Gw of a resin passage in a T-die is set to be equal to 0.5.
The apparatus for producing a long-fiber-reinforced thermoplastic resin composite according to any one of claims 1 to 4, wherein the number is from 1 to 0.3. 6. The degree of curvature Rc of at least one of the upper side and the shorter side at the exit of the resin passage in the T-die is 0.01 to
The apparatus for producing a long-fiber-reinforced thermoplastic resin composite according to any one of claims 1 to 5, which is 0.05. 7. An apparatus in which an opening impregnation tank is connected to the downstream side of an extruder, wherein a resin passage in a T-die connected between a downstream end of the extruder and an upstream end of the opening impregnation tank is provided. It has an outlet cross-sectional area larger than the inlet cross-sectional area, and the decreasing gradient Gv of the resin passage in the T-die is 0.01 to 0.1, and the widening gradient Gw of the resin passage in the T-die is 0.1. 1 to 0.
The apparatus for producing a long-fiber-reinforced thermoplastic resin composite according to any one of claims 1 to 6, wherein