JPH10278212A - Production of composite laminate - Google Patents

Abstract

PROBLEM TO BE SOLVED: To eliminate the remaining of air bubbles in the adhesive layer of a composite laminate. SOLUTION: At least two laminating materials A are bonded through a film-shaped adhesive B to produce a composite laminate D. In this case, a laminating process P1 alternately laminating the laminating materials A and the film like adhesive B to obtain a laminate raw material C, a degassing and bonding process P2 applying electromagnetic wave heating to the laminate raw material C obtained in the laminating process P1 in reduced pressure environment to mutually bond the laminated laminating materials A and an air supply process P3 supplying air to the reduced pressure environment after the completion of the degassing and bonding process P2 to return the reduced pressure environment to atmospheric pressure environment are provided.

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 composite laminate in which a transparent plate glass or a transparent synthetic resin plate is formed in a plurality of layers with an adhesive layer interposed therebetween.

[0002]

2. Description of the Related Art A composite laminate is a material obtained by combining a plurality of materials having different properties, and a composite having a characteristic superior to that of a single material is obtained. Currently, it is being actively studied in various fields, and some of them have already been put to practical use.

[0003] Conventionally, a plate-like composite laminate as described above has
An adhesive is applied to the surface of a predetermined material (substrate), and another substrate is superimposed on the substrate to which the adhesive is applied and then naturally cured, or a forced curing treatment by external heating is performed. Although it was manufactured by applying, such a method takes a long time to obtain a product, not only low productivity, but also when the external heating is performed, heat reaches the adhesive in the laminate Before passing through the layer of the base material, the heating efficiency of the adhesive becomes worse,
There has been a problem that the substrate may be adversely affected by heat.

Therefore, in recent years, a film made of a synthetic resin having thermoplasticity is used as an adhesive, and a laminate is formed by interposing the film-like adhesive between the base materials to form an electric vibration such as a high frequency. Attention has been focused on a method of manufacturing a plate-like composite laminate in which the adhesive in the laminate is heated and melted by using the adhesive, thereby exerting an adhesive function on the film-like adhesive.

As a method for producing a plate-like composite laminate utilizing such electric vibration, Japanese Patent Application Laid-Open Nos. 3-34850, 3-36663, and 62-873 have been disclosed.
No. 25, JP-A-6-293076, JP-A-6-293076
Japanese Patent Application Laid-Open Nos. 293077, 6-298549 and 6-336909 are known.

[0006]

However, when producing a transparent composite laminate by laminating a transparent glass or a transparent synthetic resin plate by the above-mentioned conventional method, air bubbles often occur in the adhesive layer, When air bubbles are mixed, not only does the appearance of the composite laminate deteriorate, but also the refractive index of light in that portion becomes different from that of other portions, and the quality of the composite laminate in optical applications deteriorates. Had.

Therefore, in the invention described in Japanese Patent Application Laid-Open No. 3-34850, a heat treatment is performed while removing bubbles by applying an electromagnetic wave to the laminate in a reduced pressure state. Even if applied, it is difficult to completely remove the air bubbles, and in particular, there is a problem that the air bubbles remain at the edge of the laminate. The residual air bubbles tend to become more pronounced as the size of the laminate increases.

[0008] The bubbles are generally formed by trapping the outside air during the laminating operation of the transparent glass or the like and the adhesive layer. It is considered that by overheating the edge of the laminate, a part (for example, moisture) of the adhesive layer at the edge is gasified, whereby air bubbles are particularly likely to be generated at the edge of the laminate.

The present invention has been made in view of the above situation, and has as its object to provide a method of manufacturing a composite laminate in which bubbles can be reliably prevented from remaining.

[0010]

According to the first aspect of the present invention,
A degassing / adhering step of applying electromagnetic wave heating in a reduced pressure environment to a laminated material obtained by interposing a film adhesive between the laminated materials of a plurality of laminated materials to adhere the laminated materials to each other, After the deaeration / adhesion step, an air supply step of returning the reduced pressure environment to the normal pressure environment by supplying air to the reduced pressure environment is provided.

According to a second aspect of the present invention, there is provided a laminating step in which a film-like adhesive is interposed between each of a plurality of laminated materials to obtain a laminated material, and a laminating material obtained in the laminating step. A degassing / adhering step of applying electromagnetic wave heating in a depressurized environment to bond the laminated materials to each other, and supplying air to the depressurized environment after completion of the degassing / adhering step, thereby returning the depressurized environment to a normal pressure environment. And an air supply step.

According to the first and second aspects of the present invention, the laminate raw material formed by alternately laminating via a film-like adhesive is subjected to dielectric heating or microwave heating in a degassing / bonding process under a reduced pressure environment. Is subjected to electromagnetic wave heating,
The laminated materials are bonded to each other by the melting of the film adhesive. Then, in a state where the film-like adhesive is melted, the space in which the laminate material is present is in a decompressed environment, so that the air bubbles existing in the adhesive are sucked out, and thus the air bubbles in the adhesive are removed. Is easily removed.

Next, in the air supply step after the deaeration / adhesion step, air is supplied to the decompressed environment, and the presence of the air causes the enclosed space in which the laminate material is present to become a normal pressure environment. The enclosed space, which had been low temperature due to the substantially vacuum state, was heated by the heat of the surroundings due to heat transfer and thermal convection due to the presence of air, and this heat was conversely supplied to the edge portion of the laminate material As a result, the temperature of the edge portion is raised, whereby the flowability of the molten adhesive at the edge portion of the laminate raw material is improved, and the pressure of the bubbles existing at the edge portion is increased.

Due to the improvement of the fluidity and the increase of the pressure of the bubbles, the mechanical balance of the surroundings of the bubbles existing at the edge portions of the raw material for the laminate is lost, and moreover, the edges of the raw material for the laminate are closer to the edges than the central portion. However, the bubbles move easily in the direction of the edges due to the improvement in the flowability of the adhesive, so that the bubbles move to the outside of the edge, and thereby the edges that could not be removed in the deaeration / adhesion process. Air bubbles remaining in the part are removed.

The third aspect of the present invention provides the first or second aspect.
In the described invention, a curing step is added after the air supply step.

According to the present invention, the laminated material is stabilized by leaving it to stand in the curing step to stabilize the bonding state between the laminated materials, and the film-like adhesive which has been softened by the temperature drop due to the cooling. After curing, a composite laminate in which the respective laminates are securely bonded to each other via the film adhesive is obtained.

According to a fourth aspect of the present invention, in the method for manufacturing a composite laminate according to any one of the first to third aspects, the supplied air is suctioned and removed after the air supply step, and the compressed air is returned to the reduced pressure environment. And a curing step of returning the reduced-pressure environment to the normal-pressure environment and curing after the completion of the re-aeration step.

According to the present invention, when the temperature of the edge of the film adhesive becomes significantly higher than a predetermined temperature, that is, the melting point of the film adhesive in the suction process, the film adhesive is thermally decomposed. Even if air bubbles are formed at the edge of the composite laminate by the decomposition gas, the decomposed gas is generated around the composite laminate in the added degassing step. Moves toward the reduced pressure environment and escapes from the adhesive in the molten state to the outside, and bubbles caused by the decomposition gas are removed.

According to a fifth aspect of the present invention, in the fourth aspect, a curing step is added after the re-supplying step.

According to the present invention, the laminated material is stabilized by allowing it to stand still in the curing step, whereby the bonding state between the laminated materials is stabilized, and the film-like adhesive which has been softened by the temperature drop due to the cooling is used. After curing, a composite laminate in which the respective laminates are securely bonded to each other via the film adhesive is obtained.

According to a sixth aspect of the present invention, in the first aspect of the present invention, in the degassing / adhering step, the laminate is not heated by a pair of electrode plates for performing dielectric heating. It is characterized in that it is abutted and clamped via a cushioning material in a pressure state.

According to the present invention, since the laminate raw material is not pressed and sandwiched by the pair of electrode plates for dielectric heating and is in a non-pressurized state, the fluidity of the adhesive in a molten state by electromagnetic wave heating is obtained. Is larger than in the case of pressurization, so that the bubbles in the molten adhesive are easily moved, and the bubbles are easily removed by suction.

[0023]

FIG. 1 is a process chart showing a first embodiment of a manufacturing process of a composite laminate to which the present invention is applied.
As shown in this figure, the manufacturing process of the composite laminate to which the manufacturing apparatus of the present invention is applied includes a lamination process P1, a deaeration / adhesion process P2, an air supply process P3, and a curing process P4.

In the laminating step P1, the laminating material A (A1, A
This is a step of sandwiching and laminating the film-like adhesive B between 2), and the film-like adhesive B is laminated on the lowermost layered material A2 placed on the carriage 5, which will be described later, and further thereon. This operation is sequentially repeated by the number of layers to be laminated, and the laminated material A is laminated on the uppermost layer, whereby a laminated body material C is obtained. Such a laminating operation is usually performed manually by an operator, but the laminating material A and the film-like adhesive B are alternately supplied onto an appropriate mounting table by using a predetermined conveying means, and the laminating operation is automatically performed. It may be made to perform it.

The laminate raw material C formed in the above-mentioned laminating step P1 is degassed and bonded in
I send it to 2. The carriage 5 may be manually driven, or may be configured to be self-propelled by driving a mounted drive motor or driving around a chain or the like.

The deaeration / adhesion step P2 is performed by using the laminate material C
Is placed in a vacuum state to remove air remaining at the boundary between the laminate material A and the film adhesive B in the laminate raw material C while applying a high frequency to the laminate raw material C. The film adhesive B is heated and melted by the dielectric heating, and the film adhesive B is melted by the melting.
To exhibit the function as an adhesive, film-like adhesive B
This is a step of bonding the laminated materials A to each other through the intermediary. Through this step, the upper and lower laminated materials A are in close contact with each other via the film adhesive B without any gap. In this step, a high-frequency welding machine 31 (FIG. 2) described later is used.

In the air supply step P3, after the deaeration process and the high-frequency application process are continued for a predetermined time in the deaeration / adhesion process P2, the vacuum environment in which the laminate material C is located is returned to the original normal pressure. This is the step of returning. The laminate raw material C becomes a composite laminate D as a final product through the air supply step P3. The processing in the air supply step P3 is performed in the high-frequency welding machine 31. By passing through the air supply step P3, the bubbles in the film adhesive B remaining at the periphery, particularly at the four corners of the laminate material C, which could not be removed in the deaeration / adhesion step P2, disappear. Thus, the composite laminate D, which is the final product, is a non-defective product having no air bubbles.

The curing step P4 is a step in which the composite laminate D obtained in the air supply step P3 is left for a predetermined time in the high frequency welding machine 31 without applying high frequency. In this step, the laminate raw material C is used to secure the bonding state between the laminate material A and the film-like adhesive B, and the composite laminate D
become. Then, the carriage 5 on which the composite laminate D is mounted is moved out of the high-frequency welding machine 31 so that the composite laminate D
From the high frequency welding machine 31 is carried out.

The composite laminate D thus obtained is
The product may be shipped as it is, or may be cut into a predetermined size and commercialized. In this case, the composite laminate D is introduced into a cutting step (not shown) set downstream of the curing step P4. Then, in this cutting step, it is cut into a predetermined size. By applying the water jet cutting machine in the cutting step, the composite laminate D is cut accurately and reliably despite being formed by laminating hard and soft materials.

As the laminated material A, glass or a synthetic resin plate is used. As a synthetic resin for a synthetic resin plate, polyethylene (PE), polypropylene (PP), polyvinyl chloride (PVC), polystyrene (PS), acrylonitrile butadiene styrene copolymer (AB)
S), polymethyl methacrylate (PMMA), polyethylene terephthalate, polyamide (PET), polyacetal (POM), polycarbonate (PC), polyphenylene terephthalate (PPE), polybutylene terephthalate (PBT), polysulfone (PSF),
Polyether sulfone (PES), polyphenylene sulfide (PPS), polyamide imide (PAI),
Examples thereof include polyether amide (PEI), polyether ether ketone (PEEK), polyimide (PI), and polytetrafluoroethylene.

Examples of the film adhesive B include ethylene-vinyl acetate copolymer (EVA), modified EVA, synthetic rubber, polyurethane, PE, PP, PV
C, those manufactured using thermoplastic resins such as polyvinyl butyral (PVB) and ionomer resins as raw materials are employed. A film adhesive (B) is obtained by molding any of these thermoplastic resins into a film (thickness of several μm to 1 mm) according to a conventional method. It is also possible to use a film obtained by reacting and curing a reactive hot melt adhesive.

Of the above, modified EVA is particularly effective as film adhesive B. This modified EVA is EVA
Alternatively, it is a composition comprising a saponified product thereof and a copolymer of an acrylic acid ester or a vinyl ester and an unsaturated carboxylic acid, and is excellent as an adhesive for laminated glass. It is commercially available under the trademark name.

The reactive hot-melt adhesive is obtained by reacting and curing a hot-melt adhesive having a functional group via the functional group, for example, by reacting an excess polyisocyanate with a polyol. The resulting moisture-curable adhesive can be mentioned. The prepolymer reacts with water (moisture) to form a three-dimensional crosslinked structure, thereby forming a tough film.

Hereinafter, an apparatus used in each of the above steps will be described with reference to FIGS. FIG. 2 is a partially cutaway perspective view showing the entire configuration of the embodiment of the manufacturing apparatus 1. 2 and FIGS. 3 and 4, which will be referred to later, the XX direction is referred to as the front-rear direction, the YY direction is referred to as the width direction, the -X side is referred to as the upstream side, and the + X side is referred to as the downstream side. In addition, the −Y side is referred to as a left side, and the + Y side is referred to as a right side.

As shown in FIG. 2, an apparatus 1 for manufacturing a composite laminate comprises a laminate 2 which alternately laminates a laminate material A and a film adhesive B into a laminate material C, An electromagnetic wave heating unit 3 that is provided adjacent to the downstream side and converts the laminate raw material C from the stacking unit 2 into a composite laminate D; and an electromagnetic wave heating unit that is provided downstream of the electromagnetic wave heating unit 3 and The storage material 4 for temporarily storing the composite laminate D from Step 3 until it is carried out of the system, and the laminate raw material C between the laminate 2 and the electromagnetic wave heating unit 3 and between the electromagnetic wave heating unit 3 and the storage unit 4 (Composite laminated body D) is mounted and provided so as to be able to travel, and has a basic configuration including a carriage 5. Then, the laminating process P1 is performed in the laminating unit 2, and the degassing / adhering process P2 and the air supplying process P3 are performed in the electromagnetic wave heating unit 3.

The laminated portion 2 has a rectangular base 20 in plan view including four columns 21 erected on the floor F and a table plate 22 supported by the columns 21, And a pair of rails 23 laid. The rail 23 is laid so as to communicate with rails 23, 35, and 43, which will be described later, laid on the electromagnetic wave heating unit 3 and the storage unit 4. The carriage 5 is guided by these rails 23, 35, and 43. It is possible to reciprocate between the laminating section 2 and the electromagnetic wave heating section 3 and between the electromagnetic wave heating section 3 and the storage section 4, and the laminating material C mounted on the carriage 5 is moved by the reciprocating movement. 3 and sequentially stored in the storage unit 4 to perform predetermined processing.

The carriage 5 is provided on a rectangular frame 51 having a rectangular shape in plan view, a pair of wheel shafts 52 in the front-rear direction crossing the rectangular frame 51 in the width direction, and both end portions of the wheel shafts 52. The wheels 53 guided by the rails 23, the stacked body mounting plate 54 fixed to the upper surface of the rectangular frame 51, and substantially along the outer peripheral edge of the stacked body mounting plate 54. A plurality of locking means 55 provided at equal pitch
It is comprised including. A silicon rubber plate 54b is laminated on the surface of the laminate mounting plate 54, thereby absorbing a slight bending or unevenness of the laminate raw material C placed on the laminate mounting plate 54 and C is protected. In the present embodiment, the carriage 5 does not have self-propelled means such as a drive motor, and therefore, the carriage 5 is configured to travel by pushing by an operator.

The rectangular frame 51 has a through space 51a which is surrounded by four surrounding frames and penetrates in the vertical direction.
a is attached to the rectangular frame 51 so as to cover the upper side from above. The penetration space 51a has a vertical and horizontal dimension of the laminated material A.
Is set to be larger than the vertical and horizontal dimensions.

The laminate mounting plate 54 is formed of a metal plate, and a laminate A and a film adhesive B are laminated on the surface of the laminate mount plate 54 in a predetermined number of layers via a silicon rubber plate 54b. The peripheral portion 54a of the stacked body mounting plate 54 is slightly protruded from the peripheral portion of the rectangular frame 51, and a plurality of locking means 55 are provided at substantially equal pitches along the protruded peripheral portion 54a. Is provided.

As shown in FIG. 3, the locking means 55 includes a bracket 55a which is fixed by welding or the like so as to protrude outward on the back surface side of the peripheral portion 54a of the stacked body mounting plate 54, An actuator 55b attached to the back side of the bracket 55a, an operation rod 55c protruding upward from the actuator 55b through the bracket 55a, and an operation rod 55
and a locking claw 55d attached to the upper end of the operating rod 55c so as to extend in the radial direction of the operating rod 55c.

The actuator 55b is configured to move the operation rod 55c up and down and to rotate around the axis. When the operation rod 55c is protruded upward, the locking claw 55d is set to the lock release posture parallel to the peripheral edge 54a of the stacked body mounting plate 54, and when the operation rod 55c is lowered, When the tip of the locking claw 55d is substantially 9
It is set to the locking posture rotated by 0 °.

The electromagnetic wave heating section 3 includes a high frequency welding machine 31 provided adjacent to and downstream of the laminating section 2, and a high frequency oscillator 37 for supplying high frequency to the high frequency welding machine 31.
And pressure adjusting means 38 for adjusting the pressure in the bonding space.

The high frequency welding machine 31 includes a pair of inverted U-shaped portal structures 31a erected on the floor F in the width direction.
A ceiling plate 31d extended between the beam members 31b above the gate-shaped structure 31a, and a horizontally arranged upper electrode plate which is moved up and down by driving the first cylinder device 321 supported by the ceiling plate 31d. 32, a horizontally arranged laminated body surrounding member 33 which is moved up and down by driving the second cylinder device 331 supported by the ceiling plate 31d, and is guided by each of the columns 31c of the gate-shaped structure 31a. Cylinder device 341
And a lower electrode plate 36 provided on the floor F so as to face the upper electrode plate 32.

FIGS. 3 and 4 are partially cutaway perspective views showing one embodiment of a main part of the high frequency welding machine 31. FIG.
The cart 5 on which the laminate material C is mounted is a high-frequency welding machine 3
FIG. 4 shows a state immediately after being introduced into the rack 1 and a state in which a closed space surrounding the laminate raw material C is formed on the laminate mounting plate 54 of the cart 5. 5 is a sectional view taken along line WW of FIG. 3, and FIG. 6 is a sectional view taken along line ZZ of FIG.

As shown in FIGS. 2 to 4, the upper electrode plate 32 is formed of a metal plate having a rectangular shape in plan view in which the vertical and horizontal dimensions are set slightly larger than the maximum vertical and horizontal dimensions of the laminate material C. An intermediate plate 32b having the same planar shape as the upper electrode plate 32 is provided on the upper portion thereof through a predetermined number of connection rods 32a. On the other hand, the first cylinder device 321 includes a pair of cylinders 322 in the front-rear direction fixed to the ceiling plate 31d (FIG. 1) in a penetrating state, and a piston that protrudes and retracts from each cylinder 322 by hydraulic pressure from a hydraulic unit (not shown). Rod 32
The lower end of each piston rod 323 is connected to the intermediate plate 32b. Therefore, by making the intermediate plate 32b protrude and retract by the driving of the first cylinder device 321,
The upper electrode plate 32 includes an intermediate plate 32b and a connecting rod 32a.
Up and down through.

On the surface of the intermediate plate 32b, four slide rods 324 are provided upright at four corners. Each of these slide rods 324 is slid through the ceiling plate 31d as shown in FIG. 2, thereby preventing the upper electrode plate 32 from oscillating in the width direction and the front-rear direction. Has become stable.

The laminate surrounding member 33 includes a rectangular annular frame 33a having a rectangular shape in plan view, and a flange 33 projecting outward from the lower edge of the rectangular annular frame 33a.
b, a flat silicon rubber plate 33c stretched on the back side of the rectangular annular frame 33a so as to cover the through space.
Are formed. Such a silicon rubber plate 33
The thickness dimension of the flange portion 33b is set such that c is flush with the bottom surface of the flange portion 33b in a state of being stretched over the rectangular annular frame 33a.

The vertical and horizontal dimensions of the flange portion 33b are set to be the same as the vertical and horizontal dimensions of the peripheral portion 54a of the stacked body mounting plate 54, whereby the stacked body surrounding member 33 is placed on the stacked body mounting plate 54. Are overlapped, the end faces of the flange portion 33b and the peripheral edge portion 54a are flush with each other.

The second cylinder device 331 is provided above each of the four corners of the rectangular annular frame 33a.
Each second cylinder device 331 is provided with a predetermined intermediate connection member 31.
e, a cylinder 332 fixed to the ceiling plate 31d so as to extend in the vertical direction via the e, and a piston rod 333 protruding downward from the cylinder 332 and protruding and retracting in the vertical direction with respect to the cylinder 332. It is formed.

The lower ends of the piston rods 333 are connected to the four corners of the rectangular annular frame 33a, so that the laminated body surrounding member 33 is brought into a horizontal state by the synchronously protruding and retracting of the piston rods 333 from the cylinder 332. It is made to go up and down while maintaining.

The laminated body surrounding member 33 has intake pipes 33d provided at the four corners of the rectangular annular frame 33a and substantially at the center on the long side. Each intake pipe 33
As for d, the tip end side is projected outward from the rectangular annular frame 33a, and the base end side is the silicone rubber plate 33a.
c, the opening of which faces the surface of the stacked body mounting plate 54 below. These suction pipes 33d are connected to the suction main pipe 38c as shown in FIG.
The space between the closed space S (FIG. 6), which will be described later, and the pressure adjusting means 38 are connected via the suction pipe 33d and the suction main pipe 38c.

The elevating frame 34 has guide projections 34a projecting toward the respective columns 31c at the four corners thereof, while the respective columns 31c extend in the vertical direction corresponding to the respective guide projections 34a. Has a guide groove 310c extending,
Guide grooves 310 corresponding to the respective guide projections 34a
c in a sliding contact state with the lifting platform 34
Can move up and down while being guided by the guide groove 310c.

As shown in FIGS. 5 and 6, the elevating pedestal 34 has a through-hole 34b vertically penetrating at the center thereof, and the lower electrode plate 36 is fitted in the through-hole 34b. It is in the state of being crowded.

The third cylinder device 341 includes a cylinder 34 fixed to each column 31c so as to extend in the vertical direction.
2 and project upward from this cylinder 342,
And it is formed with a piston rod 343 provided to be able to protrude and retract in the vertical direction. The elevating gantry 34 is supported by the upper end of each piston rod 343, and moves up and down by the piston rod 343 appearing and retracting.

The elevating gantry 34 has a pair of rails 35 laid on the upper surface corresponding to the pair of rails 23 laid on the laminating section 2, and the elevating gantry 34 is located at the upper limit height position. In the raised state, the rails 23 and 35 face each other at the same height level. Therefore, by raising the lifting platform 34 to the upper limit height position with the upper electrode plate 32 and the laminate surrounding member 33 raised, the carriage 5 on the laminate 2 is moved between the laminate 2 and the electromagnetic wave heater 3. It can be made to come and go.

The lower electrode plate 36 is provided on the floor F in a frame surrounded by the four columns 31c of the electromagnetic wave heating unit 3 so as to face the upper electrode plate 32. The lower electrode plate 36 has the same plane dimensions as the upper electrode plate 32, and the vertical and horizontal dimensions are set smaller than the vertical and horizontal dimensions of the through space 51a of the truck 5. Then, in a state where the carriage 5 is moved to a predetermined electromagnetic wave heating position on the rail 35 of the electromagnetic wave heating unit 3, the lower electrode plate 36 is located immediately below the through space 51a and moves up and down by driving the third cylinder device 341. The disposition position is set so that the gantry 34 is fitted into the through space 51a by descending.

Then, with the carriage 5 being sent to the electromagnetic wave heating position of the electromagnetic wave heating section 3, the third cylinder device 34
The lowering of the elevating gantry 34 by lowering the piston rod 343 by the driving of the
The through space 51 a is fitted to the lower electrode plate 36, and the lower surface of the stacked body mounting plate 54 contacts the surface of the lower electrode plate 36 by continuing the lowering of the piston rod 343. I am trying to become. By this contact, the high frequency from the high frequency oscillator 37 is transferred to the lower electrode plate 3.
6, the stack mounting plate 54 serves as an electrode plate for the stack raw material C on the stack mounting plate 54.

Then, the trolley 5 on which the laminate raw material C is placed on the laminate mounting plate 54 is sent to the electromagnetic wave heating position of the elevating gantry 34 and the elevating gantry 34 is in the lowered position. Then, the laminate surrounding member 33 is lowered by the driving of the second cylinder device 331, and the flange 33 b abutted on each other by the operation of the locking means 55 and the peripheral edge 54 a of the laminate mounting plate 54 are mutually locked. By,
As shown in FIG. 5, the silicon rubber plate 33c is elastically deformed by the laminate raw material C and swells upward, whereby the back side of the peripheral portion of the silicon rubber plate 33c and the silicon rubber plate of the laminate mounting plate 54 An annular closed space S is formed between the peripheral portion of 54b and the upper surface side.

The pressure adjusting means 38 includes a vacuum pump 38
a, a suction main pipe 38c provided between the vacuum pump 38a and the suction pipe 33d, an outside air introduction pipe 38d branched from the suction main pipe 38c, and the outside air introduction pipe 38
d is provided with a control valve 38b.
Then, the closed space S is formed, and the control valve 38
By driving the vacuum pump 38a with b closed, the air in the closed space S is removed by suction, so that the closed space S has a vacuum environment.

In the present invention, the high frequency from the high frequency oscillator 37 is generated in a state where the inside of the closed space S is in a vacuum environment, and the lower surface of the upper electrode plate 32 is in contact with the upper surface of the silicon rubber plate 33c when the lower surface of the upper electrode plate 32 is lowered. Applied to each of the electrode plates 32 and 36,
The upper and lower laminates A are bonded to each other by the heating and melting of the film adhesive B, so that the bubbles contained in the melted film adhesive B are sucked toward the closed space in a vacuum state. It has become.

In the present invention, the upper electrode plate 3
A sensor (not shown) detects that the second cylinder 2 has come into contact with the upper surface of the silicon rubber plate 33c, and stops driving the first cylinder device 321 based on the detection signal, or releases the hydraulic pressure to release the silicon. Only the own weight of the upper electrode plate 32 is applied to the rubber plate 33c, and the pressing process is not actively performed on the laminate material C.

The reason for this is that when the raw material C being heated is pressed with a large force, the melt around the air remaining in the molten film adhesive B is strongly pressed under high pressure. In this state, it is difficult for the air to move by pushing away the strongly pressed melt, and therefore, even if the sealed space S is in a vacuum environment, This is because bubbles are not effectively removed.

As shown in FIG. 1, the storage section 4 includes a gantry 40 including four columns 41 and a table plate 42 supported by the columns 41, and the table plate 42
It is composed of a pair of rails 43 provided in the width direction. The table plate 42 is set at the same height level as the table plate 22 of the stacking unit 2, and each rail 43 is laid and set so as to correspond to each rail 35 of the lifting gantry 34 at the ascending position. In this state, the lifting gantry 3 is set in the ascending position.
The carriage 5 on the rail 35 of the storage unit 4 can be moved onto the rail 43 of the storage unit 4.

FIG. 7 is a block diagram showing an embodiment of the high-frequency oscillator 37 applied to the manufacturing apparatus 1 of the present invention. As shown in the figure, the high-frequency oscillator 37 includes a control circuit 371 for controlling the manufacturing apparatus 1 in an integrated manner, and an operation unit 3 for inputting various operation data to the control circuit 371.
72 and a high frequency generator 373 for generating high frequency power. The control circuit 371 includes the operation unit 37
Based on the operation data input via the control unit 2, the driving of each unit and the supply of power to the high-frequency generation unit 373 are controlled.

In this embodiment, the high-frequency oscillator 37
Is designed to generate a high frequency of 13.56 MHz, but the present invention is not limited to a frequency of 13.56 MHz, and can be used for heating electromagnetic waves from several MHz to several GHz. High frequencies or microwaves in the range are applicable.

The operation unit 372 includes a power switch 37
2a, a first cylinder switch 372b for switching between driving and stopping the first cylinder device 321, a second cylinder switch 372c for switching between driving and stopping the second cylinder device 331, and a second switch for switching between driving and stopping the third cylinder device 341. 3 cylinder switch 372d, locking means 5
5, a switch 372e for locking means for switching between locking and unlocking operations, a switch 372f for vacuum pump for switching between driving and stopping the vacuum pump 38a, and a control valve 38b.
And a control valve switch 372g for switching between open and closed states.

The operation signal from the power switch 372a is output to the control circuit 371 as a control signal. When the power switch 372a is turned on, the operation of the high frequency generator 373 is started, and when it is turned off, the operation of the high frequency generator 373 is stopped.

An operation signal from the first cylinder switch 372b is also output to the control circuit 371. When the first cylinder switch 372b is operated in one direction (projection side), the piston rod 323 projects and the upper electrode plate 3
2 is lowered, and when operated in the other direction (immersion side), the piston rod 323 is immersed and the upper electrode plate 32 is raised. The same applies to the second and third cylinder switches 372c and 372d, and the operation in one direction or the other direction causes the stacked body surrounding member 33 and the lift base 34 to move up and down, respectively.

When the locking means switch 372e is operated in one direction (locking side), the locking claw 55d is operated by the driving of the actuator 55b to the locking side, and when the locking means switch 372e is operated in the other direction (locking releasing side). The locking claw 55d operates to the unlocking side. Also, a vacuum pump switch 3
When 72f is turned on, the vacuum pump 38a is driven, and when it is turned off, it stops. When the control valve switch 372g is turned on, the control valve 38b opens, and when the control valve switch 372g is turned off, the control valve 38b closes.

The high frequency generator 373 includes a power supply circuit 37
4, a high-frequency generation circuit 375 that obtains electric power from the power supply circuit 374 to generate a high frequency,
5 and a matching circuit 376 provided on the output side of the control circuit 5. The power supply circuit 374 converts, for example, a commercial power supply of 220 V into a DC power supply of a predetermined level. The high-frequency generation circuit 375 is a self-excited oscillation type high-frequency generation circuit that obtains a predetermined level of DC voltage from the power supply circuit 374 and generates a required level of high-frequency energy.

Further, the matching circuit 376 is a circuit for matching the high-frequency generation circuit 375 with the laminate material C set between the pair of electrode plates 32 and 36, and
6a, a matching capacitor (not shown) is provided. The transformer 376a has an input side coil L1 and an output side coil L
The output side coil L2 has one end connected to the upper electrode plate 32 and the other end connected to the lower electrode plate 36 and the ground.

When setting the supply power, the tuning conditions may be sequentially shifted. Alternatively, if the power supply level is fixed, the power supply circuit 374 and the high-frequency generation circuit 375 may have respective predetermined ratings. When the high frequency is intermittently supplied, the heat given during the driving time is diffused into the film adhesive B during the pause time, so that the temperature distribution is made uniform, that is, the uniform heating is performed. Will be

According to the above configuration of the high-frequency oscillator 37, first, when the laminate material C is supplied to the electromagnetic wave heating unit 3, the third cylinder switch 372d is operated to the piston rod immersion side. As a result, the lifting platform 34 on which the carriage 5 is mounted on the rail 35 is lowered, and the lower surface of the stacked body mounting plate 54 comes into contact with the upper surface of the lower electrode plate 36. In this state, the second cylinder switch 372c is operated to the piston rod protruding side. As a result, the laminate surrounding member 33 descends, and as shown in FIG. 5, the rectangular annular frame 33a of the laminate surrounding member 33 comes into contact with the peripheral edge 54a of the laminate placing plate 54, and the laminate placing plate The silicon rubber plate 33c is elastically deformed so as to bulge upward by the laminate raw material C on 54, whereby an annular closed space S is formed between the silicon rubber plate 33c and the laminate mounting plate 54. .

Then, the sealed space S is
The locking means 55 is driven by the operation of the locking means switch 372e to the locking side in the state in which is formed, and the stacked flange portion 33b and the peripheral edge portion 54a of the stacked body mounting plate 54
The closed state of the closed space S is ensured by locking the contact state with the closed space S.

Then, the vacuum pump switch 372f is turned on, and the air in the sealed space S is sucked by the driving of the vacuum pump 38a, thereby creating a vacuum environment in the sealed space S. In this state, the first cylinder switch 372b
Is operated on the piston rod descending side, whereby the upper electrode plate 32 descends and comes into contact with the upper surface of the silicon rubber plate 33c. This contact state is detected by a sensor (not shown), and the first cylinder switch 372b is automatically switched to the neutral position by a control signal from the control circuit 371 based on the detection signal. The state is set in a state where pressure is not applied to the laminate raw material C via the plate 33c.

When the contact of the upper electrode plate 32 with the silicon rubber plate 33c is confirmed, the vacuum pump switch 372f is turned on, and a high-frequency voltage is applied to the upper electrode plate 32 and the lower electrode plate 36. The application state of the high-frequency voltage is continued for a predetermined time, during which the film-like adhesive B of the laminate material C is heated and melted to bond the upper and lower laminate materials A to each other.

Then, when the application of the high-frequency voltage for a predetermined time is completed, the control valve 38b is opened, and the outside air introduction pipe 38d,
Air is supplied into the closed space S through the main suction pipe 38c and the suction pipe 33d. Thereby, the inside of the sealed space S becomes a normal pressure environment, and the normal pressure environment is continued as a curing period of a predetermined time. By doing so, the temperature of the laminate material C is raised by high-frequency heating, but the environmental temperature of the closed space S, which was low due to the vacuum state, rises due to the heat transfer from the laminate material C to the air. Since the temperature of the heated air is conversely transferred to the peripheral portion of the laminate material C, the peripheral portion of the laminate material C is heated, thereby melting the peripheral portion of the laminate material C. Bubbles in the adhesive expand, and the expansion becomes a driving force and moves in a direction of low resistance, that is, in a direction from the edge of the laminate material C to the outside, and remains at the edge of the laminate material C. Bubbles in the film adhesive B are removed.

After the elapse of the curing period, the upper electrode plate 32 and the laminate surrounding member 33 are raised by operating a predetermined switch, and at the same time, the lifting platform 34 is also raised, so that the stacked stack is opened. The composite laminate D on the placing plate 54 is moved to the storage section 4 by the movement of the carriage 5, and then carried out to the next step.

Thereafter, the laminated material A and the film adhesive B
Of the composite laminate D is sequentially manufactured by repeating the supply of the composite laminate D onto the carriage 5, the transfer to the electromagnetic wave heating unit 3, the switch operation described above, and the transfer of the obtained composite laminate D to the storage unit 4. .

In this embodiment, the deaeration / adhesion step P
The application of the high-frequency voltage to the laminate raw material C and the timing of stopping the application in 2 are performed according to a preset time schedule, but a thermometer (not shown) for detecting the temperature of the closed space S is provided. The timing for the laminate raw material C may be determined each time according to the temperature detected by the meter.

The amount of heat generated by electromagnetic wave heating (W /
cm ² ) is represented by P = ((5/9) / 10 ¹² ) · f · E ² · ε · tan δ. Here, f is the frequency of the high frequency, E is the strength of the electric field (V / cm), ε is the dielectric constant, tanδ is the dielectric loss angle, and (ε × tanδ) is particularly called the dielectric loss coefficient. I have. From the above equation, the calorific value P is proportional to the square of the strength of the electric field (E ² ) and the loss coefficient (ε × tan δ), and those having a loss coefficient of 0.01 to 1 are particularly preferable as the adhesive. .

In this embodiment, the laminated material A
Is used as the glass, and the glass is a film adhesive B
Since the loss coefficient is much smaller than that, the high-frequency energy applied to the laminate material C has little effect on the laminate material A and is consumed by the self-heating of the film adhesive B. Only the adhesive B is heated and melted, and does not thermally affect the glass as in the case of external heating.

FIG. 8 is a sectional view showing an example of the film adhesive used in the present invention. As shown in this figure, a film adhesive B having a three-layer structure in which an adhesive layer b is laminated on the front and back of a thin core film a is used. In this embodiment, a PET film having a thickness of 36 μm is used as the core film a.
An ET film in which an adhesive layer b made of modified EVA is laminated on the front and back sides is employed.

By using the film adhesive B having a three-layer structure having such a core film a, the film adhesive B becomes very durable and easy to handle. In the adhesive application process, the application operation of the adhesive can be performed simply by putting the film-like adhesive B on the laminated material A without performing a troublesome operation such as coating, and the adhesive application can be performed reliably and quickly. This is extremely effective in easily applying the adhesive to the laminate A. FIG. 9 is a cross-sectional view showing one embodiment of a composite laminate D in which such a film adhesive B is employed. As shown in this figure, the composite laminate D is in a state in which the upper and lower laminates A are firmly bonded to each other by a three-layer film adhesive B.

As described in detail above, in the method for producing a composite laminate of the present invention (FIG. 1), a composite laminate D is produced by bonding at least two laminates A via a film adhesive B. A laminating process P1 in which a laminate material A and a film adhesive B are alternately laminated to form a laminate material C, and the laminate material C obtained in the laminate process P1 is heated by electromagnetic waves in a reduced pressure environment. And a degassing / adhering step P2 for adhering the laminated materials A to each other and supplying air to the depressurized environment after the degassing / adhering step P2 is completed, thereby changing the depressurized environment to a normal pressure environment Since the composite laminate D is manufactured through the returning air supply step P3, the laminate raw material C formed by alternately laminating via the film-like adhesive B in the lamination step P1 is deaerated and bonded. In step P2, electromagnetic wave heating is performed under a reduced pressure environment. This by laminate A by melt film adhesive B are bonded to each other. Then, in a state in which the film adhesive B is melted and becomes a molten adhesive, the closed space S in which the laminate raw material C is present is in a reduced pressure environment. Air bubbles are sucked out, so that bubbles in the film adhesive B are easily removed.

Next, in the air supply process P3 after the completion of the deaeration / adhesion process P2, the air is supplied into the closed space S, so that the reduced pressure environment is changed to the normal pressure environment where air is present. The enclosed space, which was low in temperature due to the vacuum state, was heated by the surrounding heat obtained by heat transfer and thermal convection in the presence of air, and this heat was conversely supplied to the edge of the laminate material C. As a result, the temperature of the edge portion is increased, whereby the flowability of the molten adhesive at the edge portion of the laminate raw material C is improved, and the pressure of the bubbles existing at the edge portion is increased.

Due to the improvement of the flowability of the molten adhesive and the increase of the pressure of the bubbles in the molten adhesive, the mechanical balance of the surroundings of the bubbles existing at the edge portion of the laminate raw material C is lost. Since the edges of the raw material C are easier to move due to the improved fluidity of the film adhesive B at the edges than at the center, the bubbles move in the direction of the edges, thereby degassing and degassing. Bubbles remaining at the edge portions that could not be removed in the bonding step P2 are removed.

In the present invention, in the degassing / adhering step P2, the laminate material C is held in a non-pressed state by the pair of high-frequency electrode plates 32 and 36 via the silicon rubber plates 33c and 54b. Therefore, the laminate raw material C is in a non-pressurized state where it is not pressed and sandwiched by the pair of electrode plates, and the fluidity of the film adhesive B in a molten state by electromagnetic wave heating is pressurized. Therefore, the bubbles in the molten adhesive are easy to move, and the bubbles are easily removed by suction.

As described above, according to the present invention, since the composite laminate D is formed without bubbles in the film adhesive B sandwiched between the adjacent laminates A, the laminate A is made of glass. In some cases, no bubbles are present in the laminated glass as the composite laminate D, and the appearance of the bubbles due to the presence of the bubbles is eliminated, and the laminated glass can be used for optical applications.

When an opaque material is used as the laminated material A, the non-uniformity of the adhesive force due to the presence of air bubbles is eliminated, so that at least two sheets adhered with the film adhesive B interposed therebetween. It becomes possible to improve the shear strength of the composite laminate D made of the laminate A.

FIG. 10 is a process chart showing a second embodiment of the manufacturing process of the composite laminate to which the present invention is applied. As shown in this figure, in the second embodiment, in the air supply process P3
A re-aeration step P3 ', in which the air supplied between the heating step P4 and the curing step P4 is removed by suction, and the reduced-pressure environment is restored, and a re-supply step P3 "for returning the reduced-pressure environment to the original normal pressure environment are provided. In the re-deaeration step P3 ', an operation of returning the closed space S (FIG. 6) once set to the normal pressure environment to the reduced pressure environment is performed by the pressure adjusting means 38 (FIG. 1). )
Is performed by closing the once opened control valve 38b and driving the vacuum pump 38a. In this way, the air in the sealed space S is sucked through the suction main pipe 38c by the driving of the vacuum pump 38a, and the inside of the sealed space S again becomes a reduced pressure environment, and the film-like adhesive on the peripheral edge of the laminate raw material C is formed. Perfection of removal of bubbles generated in B can be expected.

Then, in the second embodiment, the air supply process P
The re-deaeration step P3 ′ was interposed between the curing step P3 and the curing step P4 because the temperature of the edge portion of the laminate raw material C in the supply step P3 was too high than a predetermined temperature, and the film-like state The heat-melting state of the peripheral portion of the adhesive B is excessively advanced, and a part of the adhesive B may be decomposed to generate a decomposed gas, and bubbles resulting from the decomposed gas may be formed at the edge of the laminate material C. However, this is to remove the bubbles.

The tendency of the peripheral temperature of the film adhesive B to be too high in the air supply step P3 tends to occur when the melting point of the film adhesive B is higher than that of a standard adhesive. This is because the temperature raising process in the air supply process P3
As described above, the heat transfer using the air introduced into the closed space S as a medium is often performed, and this heat transfer is performed in a state in which strict control is difficult to be performed. This is considered to be because if this heat transfer heat treatment is to be performed on the target, the initial temperature tends to be set higher.

Specifically, when the composite laminate D is a laminated glass used indoors, the film adhesive B often has a melting point of about 70 ° C. In the case of manufacturing, the laminated glass for outdoor use may rise to near 80 ° C. when exposed to the hot summer sunshine, and to prevent the melting of the film adhesive B by this, the laminated glass for outdoor use Is usually a film adhesive B having a melting point of about 100 ° C.

The film adhesive B having such a high melting point
Is adopted, it is necessary to raise the temperature of the sealed space S to about 100 ° C. in the deaeration / adhesion step P2.
3, the temperature may exceed 120 ° C., which is the temperature at which the edge of the film adhesive B is thermally decomposed. In this case, decomposition gas is generated from the film adhesive B, and air bubbles are generated at the edge of the composite laminate D. May be formed. The re-deaeration step P3 'of the second embodiment is employed to remove such decomposed gas bubbles.
Thus, the closed space S is set to the reduced pressure environment again, whereby the air bubbles in the film adhesive B are sucked and removed in the direction of the closed space S.

Note that the above-mentioned decomposed gas bubbles are not generated only in the case of the film adhesive B having a high melting point (for example, the film adhesive B having a melting point of 100 ° C. used for the laminated glass for outdoor use). Of the film adhesive B having a low melting point (for example, the film adhesive B having a melting point of 70 ° C. used for the above laminated glass for indoor use), the temperature rise in the air supply step P3 is remarkable and greatly exceeds 90 ° C. In such a case, decomposition gas bubbles are generated. Therefore, the employment of the re-deaeration step P3 'for removing the decomposed gas bubbles is not limited to the case where the film adhesive B having a high dissolution temperature is used, and the use of the film adhesive B having a low dissolution temperature is used. It can be adopted also in the case.

When the bubble removal process for a predetermined time in the re-deaeration step P3 'is completed, the vacuum pump 38a (FIG. 2)
Is stopped and the control valve 38b is opened,
As a result, the outside air is supplied to the outside air introduction pipe 38 d and the suction main pipe 3.
8c into the closed space S through the re-supply process P
3 "is performed to set the normal pressure environment in the closed space S. Then, after the curing process P4 similar to the first embodiment in which the normal pressure environment is continued for a predetermined time is performed, the composite laminate D is formed.
Is drawn out of the electromagnetic wave heating unit 3.

As described above, the composite laminate D of the second embodiment
In the manufacturing process, the re-aeration step P3 'is interposed between the air supply step P3 and the curing step P4, and the temperature of the film adhesive B becomes too high in the air supply step P3 in which temperature control is difficult. In order to remove the decomposed gas bubbles caused by the above, it is possible to more finely remove fine bubbles that are easily generated at the peripheral portion of the composite laminate D, and the defect rate is small,
And it is extremely effective in producing a composite laminate D having a high commercial value.

[0099]

【Example】

1. Test for confirming the effect of the method of the present invention (a) Test in the case of using a composite laminate as an indoor laminated glass (Example 1) A laminate material obtained by alternately laminating a laminated material and a film-like adhesive was used. After applying a high-frequency heating for a predetermined time in a reduced pressure environment, returning to a normal pressure environment and passing a predetermined curing period, no bubbles remain in the molten film adhesive (the effect of the method of the present invention). In order to confirm, an effect confirmation test of the method according to the first embodiment was performed using the manufacturing apparatus 1 described above. This test is performed when a laminated glass for indoor use using a film adhesive B having a low melting point as the composite laminate D is obtained. The content of the test is as follows.

Types of Laminate and Film Adhesive and Laminate Structure of Laminate Raw Material Two glass plates each having a thickness of 3 mm were employed as a laminate, and the above-mentioned modified EVA was applied to the front and back of a PET film as a film adhesive. The thickness of the laminated layer is 250μm
One so-called reinforced EVA film was employed. Modified EVA laminated on the front and back of this reinforced EVA film B1
Has a melting point of about 70 ° C. These materials are 91
Cutting to 5 mm x 1830 mm to make them the same size, then laying one glass plate A 'on the lowermost layer, and stacking a reinforcing EVA film B' and another glass plate A 'on top of it. To obtain a laminated glass raw material D1 (FIG. 11) having a three-layer structure.

Test Procedure The laminated glass raw material D1 was placed on the laminated body placing plate 54 of the truck 5 shown in FIG.
Of the third cylinder device 3
The lifting platform 34 is moved down by the drive of the
4 was brought into contact with the lower electrode plate 36.

Then, the laminated body surrounding member 33 is moved down by driving the second cylinder device 331 to cover the laminated glass raw material D1 with the silicon rubber plate 33c, whereby the outer peripheral portion of the laminated glass raw material D1 is laminated with the silicon rubber plate 33c. An annular closed space S surrounded by the body mounting plate 54 is formed, and the upper electrode plate 32 is driven by the first cylinder device 321.
Was lowered, and the lower surface thereof was brought into contact with the upper surface of the silicon rubber plate 33c (the state shown in FIGS. 4, 6, and 11). After confirming this contact, the supply of the hydraulic pressure to the first cylinder device 321 was cut off so that a large compressive force was not applied to the laminated glass raw material D1.

FIG. 12 is an explanatory plan view showing a state in which the laminated glass raw material D1 is mounted between the upper and lower electrode plates 32 and 36. As shown in FIG. Air was sucked from six intake pipes 33d provided at substantially equal intervals. In this embodiment, the silicon rubber plates 33, 54
Prior to mounting the laminated glass raw material D1 in the space b, a plurality of cylindrical spacers S
1 (FIGS. 11 and 12), and the silicon rubber plate 33c
Is supported by the spacer S1, and the silicon rubber plate 33
This prevents c from clogging in the direction of the closed space S and blocking the air suction passage.

Then, the vacuum pump 38a (FIG. 1) was driven to suck and remove the air in the closed space S, and the closed space S was set to a reduced pressure environment. In this state, the high-frequency oscillator 37 is driven to apply a high-frequency voltage from the upper and lower electrode plates 32 and 36 to the laminated glass raw material D1 for a predetermined period of time. The glass sheets A 'thus adhered to each other via a reinforcing EVA film B'.

After the application of the high-frequency voltage to the laminated glass raw material D1 for a predetermined time is completed, the vacuum pump 38a
While the drive of FIG. 1 was stopped, the control valve 38b was opened to introduce air into the closed space S, and the closed space S was returned from the reduced pressure environment to the original normal pressure environment. After the continuation of the normal pressure environment for a predetermined time (curing period), the first cylinder device 321
To raise the upper electrode plate 32, and then drive the second cylinder device 331 to raise the stacked body surrounding member 33,
Subsequently, the lifting frame 34 is driven by the driving of the third cylinder device 341.
Was raised to return to the original height level, and thereafter, the cart 5 was manually moved to the storage section 4 to obtain a laminated glass E1 as a composite laminate D as a final product on the laminate mounting plate 54.
Then, the laminated glass E1 was visually observed to check whether air bubbles remained inside.

The temperature change in the closed space S from the start of applying the high frequency to the laminated glass raw material D1 to the end of the curing period was measured over time.

As a comparative example, as a laminated glass raw material D1
After the completion of the electromagnetic wave heating, a test was performed to produce a laminated glass E2 without returning the inside of the closed space S to normal pressure. The procedure in this case is the same as the above except that the vacuum pump 38a is stopped and the control valve 38b is opened after the end of the curing period.

Test Conditions The test conditions (Example 1) according to the method of the present invention and the test conditions (Comparative Examples 1 to 3) different from Example 1 were set as follows, respectively, and the laminated glass E1 was obtained by the above procedure. , E2
Was manufactured.

First, in the first embodiment, after setting the degree of vacuum in the closed space S to 730 mmHg, the supply current to the upper electrode plate 32 is initially controlled to 5.0 A, and this state is continued for 120 seconds. After that, the current was reduced to 4.0 A, and the electromagnetic wave heating was continued for 60 seconds. And 4.0A
After the electromagnetic wave heating for 60 seconds, the operation of the vacuum pump 38a was stopped, and the control valve 38b was opened, thereby returning the pressure in the closed space S to normal pressure. Then, the closed space S
The laminated glass E1 was taken out after a curing period in which the inside temperature was reduced to approximately 50 ° C.

When the laminated glass raw material D1 was sandwiched between the upper and lower electrode plates 32 and 36, the upper glass plate 32 did not press the laminated glass raw material D1. Therefore, the surface pressure received by the laminated glass raw material D1 is approximately 1 kgf / cm ² .

Next, in the first comparative example, the same surface pressure was set to 4 kgf / cm ² , and the other operations were the same as those in the first embodiment.

In Comparative Example 1, after the degree of vacuum in the closed space S was set to 730 mmHg, the upper electrode plate 3
The supply current to 2 was set to 6.0 A, which was slightly larger than that of Example 1 throughout, and this state was continued for 180 seconds.
The current supply to the upper electrode plate 32 was stopped, and the temperature was kept at the initial level of vacuum until the temperature in the closed space S became approximately 50 ° C. Further, the laminated glass raw material D1 is composed of the upper and lower electrode plates 32, 3
6, the surface pressure of the laminated glass raw material D1 in the state of being sandwiched between
3 kgf / cm ² when depressurized, 4 k when pressurized by electrode plate
gf / cm ² . Other operations were performed in the same manner as in Example 1.

In Comparative Example 2, the conditions for high-frequency heating (current supply conditions to the anode current) were the same as in Example 1, and the sealed space S was continuously depressurized 180 seconds after the start of high-frequency heating. Environment. In Comparative Example 3, both the conditions of the high-frequency heating and the conditions of the closed space S were the same as those of the example, but the pressurization by the electrode plate was continued after elapse of 180 seconds.

Test Results Table 1 shows the test results for the above Example 1 and Comparative Example.
Table 1 shows the temperature changes in the closed space S of Example 1 and Comparative Example 1 respectively.

[0115]

[Table 1]

As can be seen from Table 1, in Example 1, no bubble was present at the edge of the obtained laminated glass E1, whereas in any of Comparative Examples 1 to 3, the edge of the laminated glass E1 was obtained. The presence of small bubbles was observed in the part.

Although the reason for this is not clear, in the first embodiment, as shown in FIG. 13, after 180 seconds, the sealed space S was rapidly returned from the vacuum environment to the normal pressure environment. Flows into the closed space S, to which the convection heat and the transfer heat have not been transmitted, is heated by the convection heat and the transfer heat due to the presence of the air. The melted adhesive layer (modified EVA) of the reinforced EVA film B 'at the end portion transmitted from the outside to the outside becomes easier to flow, and the bubbles formed on the edge of the laminated glass E1 by this heating increase. It is considered to be.

That is, when the adhesive layer at the end of the laminated glass E1 becomes softer and flows more easily, the movement of bubbles due to expansion causes the adhesive to move in the direction of the softer edge. It is considered that the arriving air bubbles escape toward the closed space S.

Therefore, unless the operation of returning the inside of the closed space S to the normal pressure environment is performed as in Comparative Examples 1 and 2, a sharp rise in the temperature of the edge portion of the laminated glass E1 does not occur, so that bubbles are removed. Not done.

Further, as in Comparative Example 3, even if the sealed space S is returned to the normal pressure environment after the elapse of 180 seconds, the surface pressure of the laminated glass E1 received from the upper electrode plate 32 and the lower electrode plate 36 is large. It is considered that the flow state of the melted adhesive is hindered by the surface pressure, whereby the movement of the bubbles becomes difficult and the bubbles do not escape toward the closed space S.

(B) Test when the composite laminate is an outdoor laminated glass (Example 2) The periphery of the composite laminate D is manufactured by manufacturing the composite laminate D by the method according to the second embodiment of the present invention. An outdoor laminated glass E2 as shown in FIG. 14 was manufactured by the method of the second embodiment in order to confirm that air bubbles caused by the film-like adhesive did not remain in the portion. Laminated glass raw material D
As Example 2, three glass plates A 'similar to those in Example 1 and two high melting point EVA films B "sandwiched between these glass plates A' were used. It has a higher degree of crosslinking than the reinforced EVA film B 'used in Example 1 and has a melting point of about 100 ° C. By using such a high melting point EVA film B ″, even if the laminated glass E2 is applied under the sunshine outdoors, the laminated glass plate A ′ is not separated by the softening of the film.

The laminated glass raw material D2 obtained by alternately laminating the glass plate A 'and the high melting point EVA film B "is placed on the laminate mounting plate 54 via the upper and lower silicon rubber plates 33c and 54b as shown in FIG. The high-melting-point EVA film B ″ was melted by heat treatment by applying high frequency, and the upper and lower glass plates A ′ were bonded.

As shown in FIG. 15, conditions such as heating in the deaeration / adhesion step P2, the air supply step P3, the re-deaeration step P3 'and the curing step P4 were set as follows. That is, in the deaeration / adhesion process P2, the inside of the closed space S is set to a reduced pressure environment (vacuum degree: 710 mmHg), and the upper electrode plate 3
The anode current value to be supplied to No. 2 was set to 5.0 A, and after this current supply was continued for 530 seconds, the current value was reduced to 4.0 A in a reduced pressure environment, and this state was continued for 60 seconds.

Next, in the air supply step P3, the inside of the closed space S is returned to the normal pressure environment, this state is continued for 60 seconds, and in the next re-deaeration step P3 ', the closed space S is released.
The inside was set to a reduced pressure environment again. After this reduced pressure environment was continued until the temperature of the high melting point EVA film B ″ became sufficiently lower than the melting point, the sealed space S was returned to normal pressure, and a laminated glass E2 was obtained through a curing step P4 of about 300 seconds.

By treating the laminated glass raw material D2 under such conditions, as shown in FIG. 15, in the degassing / adhering step P2, the laminated glass raw material D2 is heated to a high melting point by a high-frequency heating of 5.0 A. The temperature was raised to about 100 ° C., which is the melting point of B ″, and this temperature was maintained for 60 seconds by high-frequency heating at 4.0 A, during which high melting point EVA was used.
The upper and lower glass plates A 'sandwiching the film B "are bonded to each other.

At this time, when air enters between the high melting point EVA film B ″ and the glass plate A ′, bubbles are formed at the peripheral portion of the laminated glass raw material D2. However, in the next air supply step P3, the air is closed. The high-melting point EVA film B ″ is fluidized by the above mechanism (heated to 120 ° C.), and air bubbles are led out into the closed space S, and the air bubbles disappear once. However, when the temperature of the high melting point EVA film B "becomes too high, it is thermally decomposed to generate a decomposed gas, and bubbles resulting from the decomposed gas are formed in the peripheral portion of the laminated glass raw material D2.

In this state, the degassing step P3 'is executed, whereby the decomposed gas bubbles are sucked from the edge of the melted high melting point EVA film B "into the closed space S under the reduced pressure environment. The bubbles formed at the periphery of are then removed. After returning to the normal atmospheric pressure environment in the re-air supply step P3 ″, the laminated glass E2 having a five-layer structure is cooled to substantially normal temperature in the curing step P4. Obtained. As a result of visually observing the laminated glass E2 thus obtained,
It was confirmed that there were no bubbles at the periphery.

[0128] 2. Other Examples of Composite Laminates Produced by the Method of the Present Invention Various composite laminates were experimentally produced by the method of the present invention. Tables 2 and 3 show examples of the manufactured products. As the film adhesive, a modified EVA having a thickness of 5 μm was formed on the front and back of a polyethylene terephthalate film having a thickness of 36 μm.
Film-shaped ones laminated so as to have a thickness of 0 μm and others shown in Tables 2 and 3 were used. Further, as the laminated material, a plate-shaped material such as a plate glass, an artificial marble plate, a PC-made plate, and a sheet-shaped material such as woven fabric, Japanese paper, and leather were used. Then, a film-like adhesive was sandwiched between these laminated materials, heated by applying a high frequency in a pressurized state, and then gradually cooled to obtain a composite laminated body.

[0129] In these tables, the laminated structure is as follows.
It is indicated as "laminate + adhesive + laminate", and when these laminates are further laminated to form a composite laminate, it is represented as "xn". In addition, GL indicates a glass plate, PC indicates a plate or film made of polycarbonate, numerals without units in front of them indicate thickness dimensions in mm, and numerals with μ indicate The thickness dimension in μm is shown. As for the film-like adhesive, the material of the core film is PET, and its thickness is 36 μm. A is an ordinary adhesive made of a thermoplastic synthetic resin in which a core film is not used, and B, C and D are other types of ordinary adhesives, respectively.

[0130]

[Table 2]

[0131]

[Table 3]

In all the composite laminates shown in Table 1, it was confirmed that the laminated materials of the respective layers were securely bonded to each other and that the strength was remarkably improved as compared with that of the single glass plate. . Also, those without using a glass plate showed good adhesion.

[0133]

According to the first and second aspects of the present invention,
A degassing / adhering step of applying electromagnetic wave heating in a reduced pressure environment to a laminated material obtained by alternately laminating the laminated material and the film adhesive to adhere the laminated materials to each other; Since the composite laminate is manufactured through an air supply step of returning the reduced-pressure environment to the normal-pressure environment by supplying air to the reduced-pressure environment after the bonding step, the film-like adhesive is used in the laminating step. The laminate raw material formed by alternately laminating the layers is subjected to electromagnetic wave heating under reduced pressure in the degassing / bonding step, and the laminated materials are bonded to each other by the melting of the film adhesive thereby. When the film adhesive is in a molten state, the space in which the laminate material is present is in a decompressed environment, whereby air bubbles present in the adhesive are easily sucked out, and Remove air bubbles Can Kusuru.

Next, in the air supply step after the completion of the deaeration / adhesion step, the reduced pressure environment is changed to a normal pressure environment by the supply of air. The enclosed space, which had been in a normal pressure environment and was low in temperature due to a vacuum state, was heated by the heat of the surroundings due to heat transfer and thermal convection in the presence of air, and this heat was conversely reduced to the end of the laminate material. The edge portion is heated by being supplied to the edge portion, whereby the flowability of the molten adhesive at the edge portion of the laminate raw material is improved, and the pressure of bubbles existing at the edge portion is increased. Can be.

Due to the improvement in fluidity and the increase in the pressure of the bubbles, the mechanical balance of the surroundings of the bubbles existing at the edges of the raw material for the laminate is lost, and moreover, the edges of the raw material for the laminate are closer to the edges than to the central portion. However, the bubbles move in the direction of the edge because the flowability of the adhesive is improved due to the improvement in the flowability of the adhesive, and thus the air bubbles remain at the edge portions that could not be removed in the deaeration / adhesion process. It is possible to reliably remove air bubbles.

According to the third aspect of the present invention, since the curing step is added after the air supply step, the laminated material is stably cooled in the curing step to stabilize the bonding state between the laminated materials, and The film adhesive which has been softened by the temperature drop due to cooling is hardened, and a composite laminate in which the respective laminates are securely bonded to each other via the film adhesive can be obtained.

According to the fourth aspect of the present invention, when the temperature of the edge of the film adhesive becomes significantly higher than the melting temperature of the film adhesive in the suction process, the film adhesive is thermally decomposed. Decomposition gas is generated, and even if new bubbles are formed at the edge of the composite laminate by this decomposition gas, the surroundings of the composite laminate are set to a reduced pressure environment in the added re-degassing step, The decomposed gas moves toward the reduced-pressure environment and escapes from the adhesive in the molten state, whereby new air bubbles caused by the decomposed gas can be removed.

According to the fifth aspect of the present invention, since the curing step is added after the re-supplying step, the laminated material is stably cooled in the curing step to allow the laminated materials to stably adhere to each other. In addition, the film adhesive which has been softened by the temperature drop due to cooling is hardened, and a composite laminate in which the respective laminates are securely bonded to each other via the film adhesive can be obtained.

According to the sixth aspect of the present invention, in the degassing / adhering step, the laminate is held between the pair of electrode plates for performing dielectric heating in a non-pressurized state via the cushioning material. As a result, the fluidity of the adhesive in the molten state due to electromagnetic wave heating is greater than in the case of pressurization, so that the bubbles in the molten adhesive are more likely to move, and the bubbles are more easily and reliably sucked. Can be removed.

[Brief description of the drawings]

FIG. 1 is a process chart showing one embodiment of a production process of a composite laminate according to the present invention.

FIG. 2 is a partially cutaway perspective view showing an entire configuration of an embodiment of a manufacturing apparatus used in the present invention.

FIG. 3 is a partially cutaway perspective view showing one embodiment of a main part of the high frequency welding machine, and shows a state immediately after a carriage on which a laminate material is mounted is introduced into the high frequency welding machine.

FIG. 4 is a partially cutaway perspective view showing an embodiment of a main part of the high-frequency welding machine, showing a state in which a closed space surrounding a laminate raw material is formed on a laminate mounting plate of a cart. I have.

FIG. 5 is a sectional view taken along line WW of FIG. 3;

FIG. 6 is a sectional view taken along line ZZ of FIG. 4;

FIG. 7 is a block diagram showing one embodiment of a high-frequency oscillator applied to the manufacturing apparatus of the present invention.

FIG. 8 is a cross-sectional view showing one example of a film adhesive used in the present invention.

9 is a cross-sectional view showing one embodiment of a composite laminate in which the film adhesive shown in FIG. 8 is employed.

FIG. 10 is a process chart showing a second embodiment of the manufacturing process of the composite laminate to which the present invention is applied.

FIG. 11 is an enlarged cross-sectional view illustrating a state of the closed space in the first embodiment.

FIG. 12 is an explanatory plan view showing a state in which a laminated glass raw material is mounted between upper and lower electrode plates.

FIG. 13 is a graph showing a time-dependent temperature change in a closed space during high-frequency heating in Example 1 and Comparative Example 1.

FIG. 14 is an enlarged cross-sectional view illustrating a state of a closed space in the second embodiment.

FIG. 15 is a graph showing a temporal change in temperature of a closed space during high-frequency heating in Example 2.

[Explanation of symbols]

 Reference Signs List A laminate material B film adhesive C laminate raw material D composite laminate P1 lamination process P2 deaeration / adhesion process P3 air supply process P3 'regasification process P3 "regasification process P4 curing process 1 manufacturing device 2 laminating section Reference Signs List 20 base 21 support 22 table plate 23 rail 3 electromagnetic wave heating unit 31 high-frequency welding machine 31a portal structure 31b beam 31c support 310c guide groove 31d ceiling plate 31e intermediate connection member 32 upper electrode plate 32a connection rod 32b intermediate plate 321 first Cylinder device 322 Cylinder 323 Piston rod 33 Laminated body surrounding member 33a Square annular frame 33b Flange portion 33c Silicon rubber plate 33d Intake pipe 331 Second cylinder device 332 Cylinder 333 Piston rod 34 Elevating stand 34a Guide protrusion 35 Rail 36 Lower electrode plate 37 High frequency oscillation 371 Control circuit 372 Operation section 373 High frequency generation section 374 Power supply circuit 375 High frequency generation circuit 376 Matching circuit 38 Pressure adjusting means 38a Vacuum pump 38b Control valve 38c Suction main pipe 38d Outside air introduction pipe 4 Storage section 40 Mount 41 Support column 42 Table plate 43 Rail 5 Dolly 51 Square frame 51a Penetrating space 52 Wheel axle 53 Wheel 54 Laminated body mounting plate 55 Locking means 55a Bracket 55b Actuator 55c Operation rod 55d Locking claw S Sealed space

 ──────────────────────────────────────────────────続 き Continuing on the front page (72) Inventor Masataka Shiro 4-14 North, Hongo-dori, Shiroishi-ku, Sapporo City Within Nippon Denden Co., Ltd. No. Yamamoto Vinita Co., Ltd. (72) Inventor Tsuneo Nagata 6-3-12 Kamishio, Tennoji-ku, Osaka City Inside Yamamoto Vinita Co., Ltd. (72) Yasuo Hashimoto 6-3-12, Kamio, Tennoji-ku, Osaka Yamamoto Vinita Shares In company

Claims (6)

[Claims] 1. A degassing method of applying electromagnetic wave heating in a reduced pressure environment to a laminate material obtained by interposing a film adhesive between each of a plurality of laminate materials to bond the laminate materials to each other.
A method for producing a composite laminate, comprising: a bonding step; and an air supply step of returning the reduced pressure environment to a normal pressure environment by supplying air to the reduced pressure environment after the completion of the deaeration / bonding step. 2. A laminating step of obtaining a laminated material by interposing a film adhesive between the laminated materials of a plurality of laminated materials, and applying electromagnetic wave heating to the laminated material obtained in the laminating process in a reduced pressure environment. A deaeration / adhesion step of applying the laminated materials to each other and supplying air to the decompression environment after the deaeration / adhesion step is completed, and an air supply step of returning the decompression environment to the normal pressure environment. A method for producing a composite laminate. 3. The method for producing a composite laminate according to claim 1, wherein a curing step is added after the air supply step. 4. A re-aeration step in which the supplied air is removed by suction after the air supply step to return to a reduced pressure environment, and after the completion of the re-deaeration step, the reduced pressure environment is returned to a normal pressure environment again. 2. An air supply step is added.
4. The method for producing a composite laminate according to any one of items 1 to 3. 5. The method for producing a composite laminate according to claim 4, wherein a curing step is added after the re-supplying step. 6. The method according to claim 1, wherein in the degassing / adhering step, the laminate is abutted and held by a pair of electrode plates for performing dielectric heating in a non-pressurized state via a buffer material. 6. The method for producing a composite laminate according to any one of claims 1 to 5.