JPH09183147A - Method for manufacturing multilayer laminate - Google Patents

Abstract

(57) Abstract: By moving two divided laminar flows symmetrically as a pair, the motion of each divided laminar flow is homogenized, and after widening and thinning, the layers are integrated. By preventing unevenness of the divided laminar flow during widening and thinning, and by further laminating and integrating two thin laminar flows, the pressing force can be evenly applied to enhance the adhesion of each layer. Thus, a method for producing a homogeneous and highly adherent multilayer laminate is obtained. SOLUTION: A laminar flow 1 in which at least two types of resin layers 2 and 3 are laminated intersects a lamination interface 4 in a longitudinal direction.
And the two divided laminar flows 6a and 6b are moved symmetrically in parallel with each other and rearranged vertically so that the laminated interfaces 4 face each other in parallel, and the divided laminar flows 6a and 6b are kept at intervals. In this state, the thin layer laminar flows 7a and 7b are formed by widening the laminated interface 4 in the extension direction of the laminated interface 4 and thinning it, and then two thin laminar flows 7 are formed.
By laminating and integrating a and 7b to form a laminated laminar flow 8 and repeating the above steps, the thin film layers are laminated in multiple layers.

Description

Detailed Description of the Invention

[0001]

BACKGROUND OF THE INVENTION 1. Field of the Invention The present invention relates to a method for producing a multilayer laminate in which different types of layers are laminated, and in particular, a multilayer laminate in which different types of thin film layers of a high molecular weight polymer are laminated and integrated. is there.

[0002]

2. Description of the Related Art Multiple extrusion molding is known as a method for producing a laminate in which high molecular weight polymers are laminated in multiple layers. In this multiple extrusion molding, a multiple composite is formed by coextruding different layers, and a laminate having the characteristics of each layer is obtained. However, in the case of co-extrusion, the thickness of each layer to be laminated is limited, and a thin film-like laminate cannot be obtained.

By the way, in Japanese Unexamined Patent Publication No. 4-278323, a laminar flow in which different types of layers are laminated is divided, rearranged and laminated, and the obtained laminated flow is thinned and further divided, laminated or thinned, A method of forming a laminated body of thin film layers by repeating this division-bonding-lamination-thinning many times has been proposed. In such a laminated body of thin film layers, since each layer is uniformly distributed in a thin layer, a composite body having characteristics different from those of the laminated body obtained by coextrusion can be obtained.

However, in such a manufacturing method, since the initial laminar flow before division is formed by coextrusion molding under relatively high temperature and high pressure, the adhesion of each layer is high, while the subsequent division and lamination are performed. Since the temperature and the pressure decrease as the cycle is repeated, the adhesion of different layers to be laminated tends to decrease. However, in the above publication, the four divided laminar flows are laminated and integrated. The pressure is not evenly applied to all the lamination interfaces, and the adhesion at all the lamination interfaces cannot be increased.

Further, in the above-mentioned publication, the four divided laminar flows do not move in the same or symmetrical manner when rearranged and laminated and integrated, and the streamline directions of the individual divided laminar flows move completely differently. Subtle motion differences occur in the divided laminar flows when they are integrated, and as a result, the layers cannot be uniformly distributed, and a uniform multilayer laminate cannot be obtained.

In particular, in the above publication, the four divided laminar flows are stacked and then expanded and thinned. However, due to the difference in the streamline direction of each divided laminar flow, there is a slight difference in movement as described above. Therefore, each layer has a biased distribution due to inertia when the width of the layer is increased, and the thickness of each layer becomes uneven. Therefore, by repeating such operations, there is a problem that nonuniformity increases, and as a result, it is not possible to manufacture a multilayer laminate having high homogeneity.

[0007]

SUMMARY OF THE INVENTION In order to solve the above-mentioned problems, an object of the present invention is to make two divided laminar flows symmetrically move as a pair to homogenize the movement of each divided laminar flow, In addition, by widening and thinning the layers and then integrating them, it is possible to prevent the heterogeneity of the divided laminar flow at the time of widening and thinning the layers. It is an object of the present invention to propose a method capable of increasing the adhesion of each layer evenly and thereby producing a multi-layer laminate which is homogeneous and has high adhesion.

[0008]

The present invention is the following method for producing a multilayer laminate. (1) a step of forming a laminar flow in which at least two types of layers are laminated, a step of forming the divided laminar flow by dividing the laminar flow at a division surface in the longitudinal direction intersecting the lamination interface, and The steps of moving the divided laminar flows symmetrically with respect to each other and rearranging the divided laminar flows at intervals, and expanding each of the divided laminar flows in the extension direction of the lamination interface while keeping a distance and thinning the layers. A method for producing a multi-layer laminate, comprising a step of forming a flow and a step of forming a laminated laminar flow by laminating and integrating two thin laminar flows. (2) A step of forming a power of 2 divided laminar flows, and two laminated laminar flows formed by rearranging the two divided laminar flows, widening and thinning, and stacking and integrating the two symmetric flows The method according to (1) above, further comprising the step of: (3) The method according to (2) above, characterized in that after the laminated laminar flow is moved, the layer is widened and thinned to be laminated and integrated. (4) The method according to any one of (1) to (3) above, wherein each step is repeated. (5) The method according to any one of (1) to (4) above, wherein the number of repetitions is 1 to 10 times.

In the present invention, examples of the layer forming the multilayer laminate include those made of a thermoplastic high molecular weight polymer. For example, thermoplastic resins and elastomers are widely used, and at least two different types having different properties are used. The seeds are combined and laminated alternately. Examples of materials for forming such a layer include polycarbonate (PC), linear low density polyethylene (LLDPE), and high density polyethylene (HDP).
E), polypropylene (PP), ethylene / cycloolefin copolymer (COC), ethylene / vinyl alcohol copolymer (EVOH), ionomer, polyesters such as polyethylene terephthalate, polyamides, and other known degradable polymers, conductive polymers , A piezoelectric polymer or the like can be appropriately selected and used.

When different types of layers are laminated, for example, EVOH
Examples of the laminated body include / PP, LLDPE / PP, and COC / PP. Further, dyes, pigments or foaming agents, fillers, stabilizers and the like may be blended in these layers. For example, a combination of a layer containing a dye (or pigment) and a layer not containing a dye (or pigment), or containing a dye (or pigment) of a different color, respectively 2
A combination of layers and the like are exemplified. Further, a combination of a layer containing a foaming agent and a layer not containing a foaming agent is exemplified.

In the method for producing a multilayer laminate according to the present invention, first, a laminar flow in which at least two kinds of different layers are laminated is formed. Since such a laminar flow is generally formed by coextrusion at a relatively high temperature and high pressure, the adhesion of each layer is high. Next, the above-mentioned laminar flow is divided at a longitudinal division surface intersecting the lamination interface to form a divided laminar flow. The most typical example is that the number of divided laminar flows is 2, but it may be a power of 2 such as 4, 8, 16 ...

The case where there are two divided laminar flows will be described. After the division, the two laminar flows are moved symmetrically with respect to each other and rearranged so as to maintain an interval. The moving direction can be any direction, and the divided laminar flows are symmetrically moved so as not to interfere with each other. By moving symmetrically, the moving distance and the moving angle of each divided laminar flow become equal, and the flow conditions of the laminar flow become equal.

Next, while maintaining the spacing, each divided laminar flow is widened in the extension direction of the lamination interface and thinned to form a thin laminar flow. At this time, by performing molding so that the cross-sectional area does not change, the bed flow velocity is kept constant. The thin laminar flow formed here preferably has the same width as the laminar flow before division and has a thickness of ½. In this case, the divided laminar flow with uniform flow conditions due to the symmetrical movement is widened and thinned under the same conditions, so that each thin laminar flow formed has the same shape and uniform laminar flow conditions. To be

Next, the thin laminar flows formed in the facing state as described above are symmetrically moved so as to be closer to each other and laminated and integrated, whereby the thin laminar flow having the same cross-sectional shape and the same flow condition. Since they are joined and integrated, a laminated laminar flow having a uniform layer shape and layer thickness is formed. In this case, since two thin laminar flows are integrally laminated, a pressing force is applied directly and uniformly as compared with the case where a large number of thin layers are simultaneously laminated, so that even when the temperature and the pressure decrease. A laminated laminar flow with excellent adhesion can be obtained.

When the widening and thinning of the divided laminar flow is performed after the lamination and integration as in the conventional case, a uniform laminated laminar flow cannot be obtained due to the uneven distribution of the laminar flow, but the lamination and integration after the widening and thinning are performed. By doing so, it is possible to simply stack and join the thin laminar flows that are widened and thinned into the same shape, and thereby obtain a homogeneous laminated laminar flow. In particular, when the multi-layer divided laminar flow is laminated and then thinned as in the conventional case, uneven distribution of the laminar flow is amplified.
Uniformity of the obtained laminated laminar flow, because the individual divided laminar flows are expanded and thinned and then laminated and integrated to prevent the uneven distribution of laminar flow and to directly and uniformly integrate the laminated laminar flows. Will be higher.

The case where the divided laminar flow is a power of 2 which is 4 or more will be described. It is preferable that the division is performed sequentially so that two divided laminar flows are always formed. After forming a power of divided laminar flows, it is also possible to divide into two pairs and perform the operations so as to move symmetrically. In any case, as described above, for each pair of two divided laminar flows, the rearrangement in which the laminar flows are symmetrically moved in parallel, the thinning and widening of the layers and the integration of the layers are performed to form the laminar flow.

The plurality of laminated laminar flow formed in this way has two
It is possible to move symmetrically one by one, rearrange them so as to keep a distance, and laminate and integrate them to obtain a further multi-layered laminar flow. In this case, the laminated laminar flow finally formed has a structure in which the thin laminar flow is laminated in multiple layers.

Further, a plurality of laminated laminar flows are symmetrically moved two by two and rearranged so as to maintain a space between them, widening and thinning are performed in the same manner as described above, and then laminated and integrated to form a laminated laminar flow. The above operation can be repeated to form a multi-layered laminar flow. In this case, a laminated laminar flow is obtained in which the thin layer laminar flow that has been widened and thinned is laminated in multiple layers.

Each of the laminated laminar flows formed as described above is further divided, rearranged, widened and thinned, and laminated and integrated to make each layer thin, and the thin film layers are laminated in multiple layers. A uniformly distributed multilayer laminate is produced.

The first laminar flow may be two layers or three or more layers, and the front side layer and the back side layer may be the same kind of layer or different kinds of layers. The initial thickness of each layer is determined so that the final laminated layer has a desired ratio. The number of layers in the initial laminar flow is preferably 2 to 10, preferably 2 to 4.
The number of repetitions of each step is preferably 1 to 10 times, preferably 2 to 6 times. The thickness of each thin film layer of the finally formed multilayer laminate is 0.01 to 500 μm, preferably 0.05 to 300 μm, and the number of laminated thin film layers is 10 to 10.
It can be 20000, preferably 20 to 5000.

In the above-mentioned manufacturing method, it is preferable to carry out the operation of each step by passing the laminar flow formed by the coextrusion molding through the molding die in the heat-softened state. In this case, if one cycle of each of the steps is performed by one molding die, each step can be repeated by connecting a plurality of molding dies of the same shape in series.

The multilayer laminate obtained as described above can be obtained as a molded product of any shape such as a film, a sheet, or a block. Then, by selecting the material of each layer, unique characteristics can be obtained by combining the respective characteristics. For example, by combining the gas barrier property and the rigidity, a molded product having a composite property of both can be obtained. In this way, the type, material, combination, number of layers, shape, etc. of each layer can be selected according to the desired characteristics of the molded product and used for the intended use.

[0023]

Embodiments of the present invention will be described below with reference to the drawings. FIG. 1 is a partially cutaway perspective view showing a method for manufacturing a multilayer laminate according to an embodiment of the present invention,
2 (a), (b), (c), (d), and (e) are sectional views taken along lines AA, BB, CC, DD, and EE of FIG. 1, respectively. ) Is a cross-sectional view corresponding to DD in the next cycle, and the cut surface in FIG. 1 is illustrated as an end surface.

In FIGS. 1 and 2, the laminar flow 1 is a flat laminar flow as shown in part A of FIG. 1 and FIG. 2 (a). Different resin layers 2 and 3 are laminated in a molten state. And moves in the direction of arrow X. The laminar flow 1 is obtained by coextrusion molding under a relatively high temperature and a high pressure, and the adhesiveness at the lamination interface 4 of the resin layers 2 and 3 is high.

The laminar flow 1 is evenly divided by a dividing surface 5 in the longitudinal direction intersecting the lamination interface to form divided laminar flows 6a and 6b. The divided laminar flows 6a and 6b symmetrically move parallel to each other in a direction intersecting with the laminating interface 4 and in a direction parallel to the laminating interface 4, and as shown in part B of FIG. 1 and FIG. The interfaces 5 are rearranged so that the interfaces 5 face each other in parallel with a vertical interval. At this time, the divided laminar flows 6 a and 6 b are symmetrically moved in parallel to be rearranged in the central portion of the original laminar flow 1. Then, since the respective moving distances, moving angles, etc. become equal, the flow conditions at the rearrangement positions become equal.

Next, the divided laminar flows 6a and 6b are widened in the extension direction of the lamination interface 4 and thinned in the state of being arranged at opposed positions and keeping a space therebetween, and the portion C in FIG. 1 and FIG. ), A thin laminar flow 7a, 7b is formed. At this time, forming is performed such that the cross-sectional areas of the divided laminar flows 6a and 6b do not change, so that the respective laminar flow rates are kept constant. The thin laminar flows 7a and 7b formed here are
It has the same width as the laminar flow 1 before the division and has a thickness of ½. In this case, the divided laminar flows 6a and 6b whose flow conditions are uniform due to the symmetrical movement are expanded and thinned under the same conditions, so that the formed laminar flows 7a and 7b have the same shape and uniform flow. Conditional laminar flow is obtained.

Next, the thin laminar flows 7a and 7b formed in the facing state as described above are symmetrically moved so as to approach each other and laminated and integrated to form a thin film having the same cross-sectional shape and the same flow condition. Since the laminar flows 7a and 7b are joined and integrated, a laminated laminar flow 8 having a uniform layer shape and layer thickness is formed as shown in part D of FIG. 1 and FIG. 2 (d). In this case, since the two thin laminar flows 7a and 7b are integrally laminated, pressing force is applied directly and uniformly as compared with the case where a large number of thin layers are simultaneously laminated and integrated, so that the temperature and the pressure are reduced. Even in this case, the laminated laminar flow 8 having excellent adhesion at the newly formed laminated interface 4a can be obtained.

When the widening and thinning of the divided laminar flows 6a and 6b are carried out after they are laminated and integrated as in the conventional case, a uniform laminated laminar flow 8 cannot be obtained due to the uneven distribution of the laminar flows, but as described above. By thinning and widening and then integrally laminating, the thin laminar flows 7a and 7b that have been widened and thinned into the same shape can be simply laminated and joined, thereby forming a uniform laminar flow 8. To be done. In particular, when the divided multi-layered flow is expanded and thinned after being laminated as in the conventional case, uneven distribution of the laminar flow is amplified. However, as described above, two divided laminar flows are expanded and thinned and then laminated and integrated. As a result, since the laminar flow is prevented from being unevenly distributed, the laminar flow 8 can be directly and uniformly pressed to be laminated and integrated, so that the obtained laminar flow 8 has higher homogeneity.

When the laminated laminar flow 8 obtained as described above is evenly divided by the new dividing surface 5a, the portion E of FIG.
Since the divided laminar flows 9a and 9b are formed as shown in (e), when the same steps of rearrangement, widening and thinning, and lamination integration as described above are repeated, as shown in FIG. 2 (f). A multilayer laminated laminar flow 9 which is further thinned and multilayered is obtained. By repeating the above steps in this manner, each layer is thinned and laminated, whereby a multilayer laminated body in which thin film layers are laminated in multiple layers and uniformly distributed is manufactured.

The above-mentioned steps are carried out in the following manner. Laminar flow 1 to D in FIG. 1 1-divided laminar flow 6a, 6b-thin laminar flow 7a, 7b-
Mold 1 having a resin flow path corresponding to the shape of the laminated laminar flow 8
Coextrusion molding can be continuously performed by passing the laminar flow 1 through 0 in a heat-softened state. Then, a plurality of molding dies 10a having the same shape are connected in series and each step is repeated to continuously manufacture a multilayer laminate.

FIG. 3A is a plan view showing a manufacturing method according to another embodiment, and FIG. 3B is a front view thereof. In this embodiment, an example is shown in which the laminar flow 1 moving in the Y direction is divided into four to widen and thin the layers and integrate the layers.

First, the laminar flow 1 is divided into divided laminar flows 6c and 6d by the central dividing surface 5a, and they are symmetrically translated in a direction away from each other in the extension direction of the lamination interface 4. Evenly divided into two, and two pairs of divided laminar flows 6a, 6
Divide into b. Two pairs of split laminar flows 6a and 6b are shown in FIGS.
In the same manner as in the above case, the layers are symmetrically translated in a direction intersecting with the lamination interface 4 and in a direction parallel to the lamination interface 4, and rearranged so as to face each other with a vertical gap, and then widened to be a thin layer. Laminar flows 7a and 7b are formed.

The thin laminar flows 7a and 7b are symmetrically moved in a vertically approaching direction to be laminated and integrated to form a pair of laminated laminar flows 8a and 8b. At this time, since the pressing force is applied directly and evenly, the adhesion of the newly formed laminated interface 4a becomes high. Laminar laminar flow 8 thus formed separately
a and 8b are moved in parallel in a direction intersecting with the lamination interface 4a and in a direction parallel to each other, and are rearranged in parallel to each other at parallel intervals with a vertical gap therebetween, and then widened and thinned to form a thin laminar flow 7c, 7d.
To form The thin laminar flows 7c and 7d are moved in parallel in the vertical direction to be laminated and integrated to form a multilayer laminated laminar flow 9.
At this time, since the pressing force is applied directly and evenly, the adhesion at the newly formed interface 4b is high.

The multi-layered laminated laminar flow 9 thus obtained is divided into divided laminar flows 9c and 9d by the dividing surface 5c, and divided, rearranged, widened and thinned, laminated integrated, rearranged and widened and thinned in the same manner as described above. By repeating the steps of forming and laminating, the respective layers are further thinned and laminated, whereby a multilayer laminated body in which thin film layers are laminated in multiple layers is manufactured.

In the manufacturing method shown in FIG. 3, the laminar flow 1 is passed through a mold having a resin flow path from the laminar flow 1 to the formation of the multi-layered laminar flow 9 in a heat-softened state. Can be formed, and by connecting a large number of such molds in series, it is possible to continuously manufacture a multi-layer laminated body in which a large number of thin film layers are laminated. The divided laminar flows 6a and 6b, the laminated laminar flows 8a and 8b, and the like in FIG. 3 are actually twisted laminar flows, but in FIG. 3, for simplification, they are translated in the width direction while keeping the same plane. Is illustrated in.

In the example of FIG. 3, the laminated laminar flows 8a and 8b are formed, and then the thin laminar flows 7c and 7d are formed by widening and thinning. , 8b
Can be directly laminated and integrated. In this case, when the divided laminar flows 6a and 6b are widened and thinned, they are widened to the width of the original laminar flow 1 and thinned to a thickness of 1/2 of FIG. 3 to form the thin laminar flows 7a and 7b. , A multi-layered laminar flow 9 having a width and layer thickness equivalent to FIG. 3 is formed. At this time, since it is difficult to translate the wide thin laminar flows 7a and 7b in the width direction, the divided laminar flows 6a and 6b can be rearranged in advance so as to overlap each other in the vertical direction.

In each of the above methods, a pair of divided laminar flows are symmetrically translated in parallel, and the treatment is performed under the same conditions. For this purpose, the respective layers are joined and integrated under equal conditions, and a uniform multilayer laminate having high interlayer adhesion is manufactured.

Although two divided laminar flows are formed in sequence in FIG. 3, they may be formed simultaneously. In this case, two pieces may be moved in a symmetrical movement. The number of divisions is 2 ⁿ
If (n is a natural number), it is possible to perform the above two processings. The divided laminar flows 6c and 6d may be moved vertically to be separated, and the widening and thinning may be performed in a state where they do not face each other in parallel.

In the above-mentioned multilayer laminate, by combining the materials of the resin layers 2 and 3 arbitrarily, unique characteristics in which the respective characteristics are combined can be obtained. For example, by combining a resin having a gas barrier property and a resin having rigidity, a composite property of the both can be obtained, and it can be used for a container, a packaging material and other applications.

In the above-mentioned multi-layer laminate, the lamination interface 4 of the resin layers 2 and 3 has high adhesiveness by coextrusion molding, and the interface to be subsequently joined is the joining of two thin laminar flows. ,
The pressing force is applied directly and evenly, showing high adhesion. Therefore, the interlayer adhesion of the resin layers constituting the multi-layer laminate is increased, each layer is uniformly distributed, and the characteristics are homogenized. In the above embodiment, the example of the two resin layers for the laminar flow 1 is shown, but three or more layers may be used.

[0041]

As described above, according to the present invention, a laminar flow in which at least two layers are laminated is divided, two divided laminar flows are moved symmetrically to each other and rearranged, and a space is maintained. In the state of widening and thinning, the two thin laminar flows are laminated-The motion of each divided laminar flow is homogenized, and after the widening and thinning is performed, the layers are integrated into a single layer to widen and thin the layers. By preventing non-homogeneity of the divided laminar flow and further laminating and integrating two thin laminar flows, the pressing force can be evenly applied to enhance the adhesion of each layer. High multi-layer laminates can be produced.

[Brief description of the drawings]

FIG. 1 is a partially cutaway perspective view showing a method for manufacturing a multilayer laminate according to one embodiment.

2 (a), (b), (c), (d), and (e) are AA, BB, CC, DD, and EE of FIG. 1, respectively.
A sectional view, (f) is a sectional view corresponding to DD in the next cycle.

3A and 3B show another embodiment, FIG. 3A is a plan view, and FIG.
Is a front view.

[Explanation of symbols]

1 Laminar flow 2, 3 Resin layer 4, 4a, 4b Lamination interface 5, 5a, 5b, 5c Divided surface 6a, 6b, 6c, 6d, 9a, 9b, 9c, 9d Divided laminar flow 7a, 7b, 7c, 7d Thin Laminar flow 8, 8a, 8b Laminated flow 9 Multilayered laminated flow 10, 10a Mold

Claims (5)

[Claims] 1. A step of forming a laminar flow in which at least two kinds of layers are laminated, and a step of forming the divided laminar flow by dividing the laminar flow at a division surface in a longitudinal direction intersecting a lamination interface. The steps of moving the divided laminar flows symmetrically with respect to each other and rearranging the divided laminar flows at intervals, and expanding each of the divided laminar flows in the extension direction of the lamination interface while keeping a distance and thinning the layers. A method for producing a multi-layer laminate, comprising: a step of forming a laminar flow; and a step of laminating and integrating two thin laminar flows to form a laminated laminar flow. 2. A step of forming a power of 2 divided laminar flows, and a laminar laminar flow formed by arranging the two divided laminar flows by rearranging, widening and thinning, and laminating and integrating the divided laminar flows two by two. And a step of moving and stacking them to integrate them.
The described method. 3. The method according to claim 2, wherein the laminated laminar flow is moved and thinned after the movement so as to be laminated and integrated. 4. The method according to claim 1, wherein each step is repeated. 5. The method according to claim 1, wherein the number of repetitions is 1 to 10 times.