JP2006273705A - Double-glazed unit - Google Patents

Abstract

<P>PROBLEM TO BE SOLVED: To provide a double-glazed unit which satisfies all required characteristics such as gas barrier property, shape retainability, formability and the like by only a spacer without using a secondary seal material and which is free from the problem of curing the seal material and good in productivity, and to provide a method for producing the same. <P>SOLUTION: In the double-glazed unit 1, a hollow layer 5 is formed by holding glass sheets 2, 3 at a prescribed interval by using a rubber spacer 4 containing (A) an isobutylene-based block copolymer having an alkenyl group at the terminal, (B) a thermoplastic resin and (C) a compound having at least two hydrosilyl groups in the molecule, and having hot melt adhesiveness. The production process of the double-glazed unit 1 can be made simple and thereby, the double-glazed unit 1 is good in the productivity because the rubber spacer 4 functioning as the seal material high in the adhesive force for a long period, the shape retainability and the gas barrier property, and excellent in the hot melt adhesiveness is used. <P>COPYRIGHT: (C)2007,JPO&INPIT

Description

  The present invention relates to a multilayer glass using a rubber-like spacer having excellent gas barrier properties, particularly excellent hot-melt adhesiveness, and a method for producing the same as a spacer.

  The double-glazed glass is a glass having high heat insulation properties, and has recently been attracting attention from the viewpoint of energy saving, and the demand is increasing. Most of the present multi-layer glass includes two or more glass plates, for example, two glass plates 2 and 3 through a metal spacer 14 such as aluminum filled with a desiccant d as shown in FIG. The hollow layer 5 is formed between the glass plates 2 and 3 so as to face each other. And by interposing the primary sealing material 15 between the glass plates 2 and 3 and the metal spacer 14, the hollow layer 5 is shielded from the outside air, and the inner surfaces of the peripheral edges of the glass plates 2 and 3 facing each other A gap (concave portion) 16 constituted by the outer peripheral surface of the spacer 14 is sealed with a room temperature curing type secondary sealing material 17 typified by polysulfide or silicone.

  Until now, in the manufacturing process of the double-glazed glass, various improvements in productivity by simplification or automation, and thus cost reduction have been studied. For example, a method using a spacer made of a resin composition kneaded with a desiccant instead of a metal spacer has been proposed. However, regardless of the type of spacer used, a multilayer glass using a room temperature curable sealing material requires a long period of time for curing the sealing material after the multilayer glass is manufactured. Therefore, there is a problem that the product cannot be shipped until the curing is completed.

  Therefore, from the viewpoint of lowering the cost of the double-glazed glass and simplifying the manufacturing process, a partially vulcanized rubber is used as the spacer, and a molded product made of a resin kneaded with a desiccant is used as a spacer and sealing material, and is cured at room temperature. There has been proposed a method for producing a multi-layer glass without using a mold secondary sealing material (Patent Document 1). However, the spacer resin using partially vulcanized rubber has insufficient hardness, and it is difficult to maintain the shape of the multilayer glass with a spacer made of such a resin alone.

  Moreover, it has a hardness of 95 ° JIS A hardness obtained by kneading a desiccant into a hard resin that can be formed by extrusion, for example, a vinyl chloride resin or a thermoplastic resin such as hot melt butyl that has been increased in hardness by adding silica gel. Multi-layer glass using a material as a spacer / sealant is known (Patent Document 2). However, when a material having a JIS A hardness of 95 ° is used as a spacer or sealing material for double-glazed glass, a large stress is applied to the sealing portion or glass plate of the double-glazed glass, and the sealing portion is peeled off. In addition, there are problems such as the occurrence of glass cracks in the multilayer glass itself.

  As a method for preventing the breakage of the multilayer glass, there is a method of producing a multilayer glass without using a room temperature curing type secondary sealing material, using a resin composed of butyl rubber and crystalline polyolefin as a spacer and sealing material. It has been proposed (Patent Document 3). However, since this composition uses butyl rubber with cold flow properties as a main component, there is a problem in terms of long-term durability depending on the intended use. Arise.

Furthermore, a triblock copolymer composed of a block composed of an isobutylene unit and two types of blocks composed of an aromatic vinyl compound unit is used for a multilayer glass as an elastic sealing material (Patent Document 4). The use of a thermoplastic elastomer composition having a dispersed phase composed of dynamically crosslinked rubber in a thermoplastic resin continuous phase as a sealing material / spacer for double-glazed glass has been proposed (Patent Document 5). . Since these compositions have high gas barrier properties and no cold flow properties, deformation of the sealing material such as the composition mainly composed of butyl rubber described in Patent Document 3 can be suppressed. However, since the melt viscosity in the temperature range for hot-melt adhesion to the glass plate is high, there is a problem in that sufficient adhesive force cannot be obtained, there is a problem in terms of long-term durability, and peeling of the seal portion occurs.
Japanese Examined Patent Publication No. 61-20501 Japanese Unexamined Patent Publication No. 7-17748 JP-A-10-114552 Special table 2003-506557 gazette JP 2000-119537 A

  Thus, at present, there is no known multilayer glass that satisfies all of the properties required for multilayer glass, such as life, shape maintenance, and formability, without using a secondary sealing material. . Therefore, an object of the present invention is to solve the problem of curing that takes a long time after production, and to use a multi-layer glass using a spacer that functions as a sealing material having a long-term adhesive force, shape maintenance, and high gas barrier properties, and It is in providing the manufacturing method.

  As a result of intensive studies, the present inventors have adopted the rubber spacer comprising a specific isobutylene-based polymer, a thermoplastic resin, and a sealing material composition having a hot melt adhesive containing a hydroxyl group. The present invention that can achieve the object has been completed.

  That is, the multi-layer glass according to the present invention is configured such that a plurality of glass plates are opposed to each other at a predetermined interval via a spacer provided on a peripheral portion of the glass plate so as to form a hollow layer therebetween. In the multi-layer glass, the spacer contains an isobutylene polymer (A) having an alkenyl group at the terminal, a thermoplastic resin (B), and a compound (C) having at least two hydrosilyl groups in the molecule. It is a rubber-like spacer having melt adhesion.

  In a preferred embodiment, the rubber spacer is a multilayer glass containing a compound (D) having a carbon-carbon unsaturated bond functional group which is different from the component (A).

  As a preferred embodiment, the carbon-carbon unsaturated bond functional group-containing compound (D) further includes an epoxy group, an alkoxy group, a radical polymerizable unsaturated group, a carboxyl group, a carboxylic acid anhydride group, a halogen atom, And a multi-layer glass having at least one functional group selected from the group consisting of alkoxysilyl groups.

  As a preferred embodiment, the rubber spacer is a multilayer glass further containing a nitrogen atom-containing compound (E).

  As a preferred embodiment, a multilayer in which the isobutylene polymer (A) having an alkenyl group at the terminal contained in the rubber spacer is crosslinked with a compound (C) having at least two hydrosilyl groups in the molecule. It is glass.

  As a preferred embodiment, the thermoplastic resin (B) contained in the rubber spacer is a thermoplastic elastomer, polyethylene, polypropylene, ethylene-α olefin copolymer, polyisobutylene, isobutylene-isoprene copolymer (butyl rubber). , Chlorinated butyl, brominated butyl, isobutylene- (p-methylstyrene) copolymer, and at least one selected from the group consisting of brominated products of isobutylene- (p-methylstyrene) copolymer It is.

  In a preferred embodiment, the thermoplastic elastomer is a multi-layer glass which is a styrene thermoplastic elastomer and / or a urethane thermoplastic elastomer.

  As a preferred embodiment, the styrenic thermoplastic elastomer is composed of a polymer block (a) having an aromatic vinyl compound as a constituent monomer and a polymer block (b) having isobutylene as a constituent monomer. It is the multilayer glass which is the isobutylene type block copolymer (B1) which becomes.

  A preferred embodiment is a double-glazed glass characterized in that a resin spacer is further provided on the inner peripheral side and / or outer peripheral side of the rubber spacer.

  As a preferred embodiment, the resin spacer is a multi-layer glass made of a resin composition containing 20% by weight or more of a desiccant.

  A preferable embodiment is a double-glazed glass characterized in that a sealing material made of a moisture-permeable hot melt resin containing a desiccant is provided on the inner peripheral side of the rubber spacer.

  As a preferred embodiment, a multilayer glass characterized in that a metal spacer is further provided on the inner peripheral side and / or the outer peripheral side of the rubber spacer.

  In addition, the method for producing a multi-layer glass according to the present invention includes an isobutylene polymer (A) having an alkenyl group at the terminal, a thermoplastic resin (B), and a compound (C) having at least two hydrosilyl groups in the molecule. A hot melt adhesive resin composition containing the glass plate is extruded into a predetermined spacer shape on the inner surface of the peripheral edge of the glass plate, and the other glass plate is pressure-bonded to the glass plate on which the spacer is formed. The glass plates are arranged to face each other at a predetermined interval through the spacer provided at the peripheral edge of the glass plate so as to form a hollow layer therebetween.

  In addition, another method for producing a multilayer glass according to the present invention includes an isobutylene polymer (A) having an alkenyl group at the terminal, a thermoplastic resin (B), and a compound having at least two hydrosilyl groups in the molecule ( A spacer having a predetermined shape is molded with a hot melt adhesive resin composition containing C), the spacer is bonded onto the inner surface of the peripheral edge of the glass plate, and the glass plate to which the spacer is bonded The glass plates are pressure-bonded, and the two glass plates are arranged to face each other at a predetermined interval via the spacer provided on the peripheral edge of the glass plate so as to form a hollow layer therebetween.

  The multi-layer glass according to the present invention includes a hot melt containing an isobutylene polymer (A) having an alkenyl group at a terminal, a thermoplastic resin (B), and a compound (C) having at least two hydrosilyl groups in the molecule. Since it is made of a resin composition having adhesiveness, a rubber spacer having excellent gas barrier properties and rubber elasticity, long-term durability and excellent hot-melt adhesiveness is used, so that the manufacturing process can be simplified.

  When the rubber spacer further contains a compound (D) having a carbon-carbon unsaturated bond functional group, which is different from the component (A), at least two hydrosilyl groups in the molecule. One hydrosilyl group of the compound (C) having a group is bonded to the terminal alkenyl group of the isobutylene polymer (A), and the other hydrosilyl group is a compound having a carbon-carbon unsaturated bond functional group (D ), The resin composition has sufficient adhesion durability, and the shape maintaining property and long-term durability of the multilayer glass are improved.

  Further, the carbon-carbon unsaturated bond functional group-containing compound (D) is an epoxy group, an alkoxy group, a radical polymerizable unsaturated group, a carboxyl group, a carboxylic acid anhydride group, a halogen atom, and an alkoxysilyl group. When having at least one functional group selected from the group consisting of the above, the adhesiveness of the resulting resin composition is enhanced, the hot melt adhesiveness of the rubber spacer is improved, the shape maintenance of the multilayer glass, and the long-term durability Improves.

  When the rubber spacer further contains a nitrogen atom-containing compound (E), the hot-melt adhesiveness and long-term adhesion retention of the resin composition are improved, and it has an appropriate hardness, Cracking is also prevented.

  When the isobutylene polymer (A) having an alkenyl group at the terminal contained in the rubber spacer is crosslinked with a compound (C) having at least two hydrosilyl groups in the molecule, the rubber spacer has a shape. Excellent maintainability.

  The thermoplastic resin (B) contained in the rubber spacer is thermoplastic elastomer, polyethylene, polypropylene, ethylene-α olefin copolymer, polyisobutylene, isobutylene-isoprene copolymer (butyl rubber), chlorinated butyl, bromine. When the rubber spacer is at least one selected from the group consisting of butyl bromide, isobutylene- (p-methylstyrene) copolymer, and bromide of isobutylene- (p-methylstyrene) copolymer, the rubber spacer is hot-melt adhesive The property is good.

  When the thermoplastic elastomer is a styrene-based thermoplastic elastomer and / or a urethane-based thermoplastic elastomer, the hot melt adhesiveness of the rubber spacer becomes better.

  An isobutylene block copolymer comprising the polymer block (a) having an aromatic vinyl compound as a constituent monomer and the polymer block (b) having an isobutylene as a constituent monomer. The hot melt adhesiveness of the coalesced (B1) and the rubber spacer is further improved, and further, the gas barrier property is excellent.

    The double-glazed glass in which resin spacers are further provided on the inner peripheral side and / or the outer peripheral side of the rubber spacer will be more excellent in long-term durability.

  The double glazing made of the resin composition in which the resin spacer contains 20% by weight or more of the desiccant can prevent the hollow layer sandwiched between the glass plates of the double glazing from being clouded by moisture.

  The multilayer glass provided with a sealing material made of a moisture-permeable hot melt resin containing a desiccant on the inner peripheral side of the rubber spacer is that the hollow layer sandwiched between the glass sheets of the multilayer glass is clouded by moisture. Can be prevented.

  Multi-layer glass with metal spacers installed on the inner and / or outer peripheral side of the rubber spacer is excellent in shape maintenance and long-term durability, and the thickness of the rubber spacer can be reduced. As well as the production of large double glazing.

  According to the method for producing a double-glazed glass according to the present invention, a plurality of glass plates are bonded by hot-melt adhesiveness of a rubber spacer and bonded by cooling of the rubber spacer. Is not required, the manufacturing process is simplified, and the multilayer glass can be manufactured at low cost.

  The multilayer glass according to the present invention has a plurality of glass plates, for example, spacers on the peripheral portions of the glass plates 2 and 3 so that the two glass plates 2 and 3 form a hollow layer 5 as shown in FIG. 4 are arranged to face each other at a predetermined interval. In the double-glazed glass 1 of the present invention, the spacer 4 includes an isobutylene polymer (A) having an alkenyl group at the terminal, a thermoplastic resin (B), and a compound (C) having at least two hydrosilyl groups in the molecule. It is a rubber-like spacer which has hot-melt adhesiveness containing.

  FIG. 2 is a partial cross-sectional view of the peripheral edge portion of the multilayer glass 1 according to the first embodiment of the present invention. In the double-glazed glass 1 of this embodiment, an isobutylene polymer (A ), A rubber spacer 4 containing a thermoplastic resin (B) and a compound (C) having a hydrosilyl group. With the rubber spacer 4, the glass plates 2 and 3 are kept at a predetermined interval to form a hollow layer 5, and the peripheral portion of the multilayer glass 1 is sealed by the spacer 4.

  The spacer 4 of this embodiment is composed only of a rubber spacer, and has a function of keeping a predetermined distance between the opposing glass plates 2 and 3 of the multi-layer glass 1, gas containment (gas barrier property), and sealing a peripheral portion. It has a sealing function (sealability) and moisture permeation resistance.

  In the double-glazed glass of the present invention, the rubber spacer 4 is composed of an isobutylene polymer (A) having an alkenyl group at the terminal, a thermoplastic resin (B), and the like in order to provide the above-described gas barrier properties and sealing properties. It is produced from a resin composition containing the compound (C) having a hydrosilyl group.

  FIG. 3 is a partial cross-sectional view of the peripheral edge portion of the multilayer glass 1 according to the second embodiment of the present invention. In the multilayer glass 1 of this embodiment, the isobutylene-based polymer (A), the thermoplastic resin (on the periphery of the opposing surface side of at least two glass plates 2 and 3 that are opposed to each other at a predetermined interval ( A rubber spacer 4 containing B) and a compound (C) having a hydrosilyl group is provided, and a resin spacer 6 made of a thermoplastic resin, which will be described later, is provided on the outer peripheral side of the rubber spacer 4. By the rubber spacer 4 and the resin spacer 6, the glass plates 2 and 3 are kept at a predetermined interval, and the hollow layer 5 is formed.

  The spacer of this embodiment is composed of a rubber spacer 4 and a resin spacer 6. The rubber spacer 4 has a function of maintaining a predetermined distance between the opposing glass plates 2 and 3 of the multilayer glass 1, and gas. It has a sealing function (gas barrier property), a sealing function (sealing property) for sealing the peripheral edge, a moisture permeation resistance function, and the like, and a resin spacer 6 is provided between the glass plates 2 and 3 facing each other in the multilayer glass 1. It has a function of keeping the distance between, and imparts excellent shape maintenance and long-term durability.

  FIG. 4 is a partial cross-sectional view of the peripheral edge portion of the multilayer glass 1 according to the third embodiment of the present invention. In the multilayer glass 1 of this embodiment, the isobutylene-based polymer (A), the thermoplastic resin (on the periphery of the opposing surface side of at least two glass plates 2 and 3 that are opposed to each other at a predetermined interval ( A rubber spacer 4 containing B) and a compound (C) having a hydrosilyl group is provided, and a resin spacer 6 made of a thermoplastic resin is provided on the inner peripheral side of the rubber spacer 4. By the rubber spacer 4 and the resin spacer 6, the glass plates 2 and 3 are kept at a predetermined interval, and the hollow layer 5 is formed.

  As in the second embodiment, the spacer of this embodiment is composed of a rubber spacer 4 and a resin spacer 6, and the rubber spacer 4 has a predetermined space between the glass plates 2 and 3 facing each other. A function of keeping the distance of the gas, sealing gas (gas barrier property), sealing function to seal the peripheral portion (seal property), moisture permeation resistance function, and the like. It has a function of maintaining a predetermined distance between the glass plates 2 and 3 and imparts excellent shape maintenance and long-term durability.

  FIG. 5 is a partial cross-sectional view of the peripheral edge portion of the multilayer glass 1 according to the fourth embodiment of the present invention. In the multilayer glass 1 of this embodiment, a resin spacer 6 made of a thermoplastic resin is provided on the peripheral portion on the facing surface side of at least two glass plates 2 and 3 that are opposed to each other at a predetermined interval. Further, a pair containing the isobutylene polymer (A), the thermoplastic resin (B) and the compound having a hydrosilyl group (C) on the inner and outer peripheral sides of the resin spacer 6 with the resin spacer 6 interposed therebetween. Rubber spacers 4A and 4B are provided. By the rubber spacers 4A and 4B and the resin spacer 6, the glass plates 2 and 3 are kept at a predetermined interval, and the hollow layer 5 is formed.

  As in the second and third embodiments, the spacer of this embodiment is composed of rubber spacers 4A and 4B and a resin spacer 6. The rubber spacer 4 is a glass plate 2 facing the multilayer glass 1. 3 has a function of keeping a predetermined distance between three, sealing gas (gas barrier property), sealing function (sealing property) for sealing a peripheral portion, moisture permeation resistance function, and the like. The glass 1 has a function of maintaining a predetermined distance between the glass plates 2 and 3 facing each other, and imparts excellent shape maintenance and long-term durability. Further, when the resin spacer 6 includes a desiccant, the hollow layer 5 sandwiched between the glass plates 2 and 3 of the multilayer glass 1 is prevented from being clouded by moisture. In addition, since the spacer 6 is sandwiched between the rubber spacers 4A and 4B in this way, the spacer 6 is prevented from being tilted, and the function of maintaining the interval is ensured over a long period of time. The compositions of the rubber spacers 4A and 4B containing the isobutylene polymer (A) and the thermoplastic resin (B) may be the same or different.

  FIG. 6 is a partial cross-sectional view of the peripheral edge portion of the multilayer glass 1 according to the fifth embodiment of the present invention. In the multilayer glass 1 of this embodiment, the isobutylene-based polymer (A), the thermoplastic resin (on the periphery of the opposing surface side of at least two glass plates 2 and 3 that are opposed to each other at a predetermined interval ( A rubber spacer 4 containing B) and a compound (C) having a hydrosilyl group is provided, and a sealing material 7 made of a moisture-permeable hot melt resin containing a desiccant is provided on the inner peripheral side of the rubber spacer 4. It has been. By the rubber spacer 4, the glass plates 2 and 3 are kept at a predetermined interval, and the hollow layer 5 is formed. Further, the inner peripheral side of the rubber spacer 4 is sealed by the sealing material 7.

  The spacer of this embodiment is composed of a rubber spacer 4 and a sealing material 7, and the rubber spacer 4 has a function of keeping a predetermined distance between the opposing glass plates 2 and 3 of the multi-layer glass 1, and contains gas. (Gas barrier property), a sealing function (sealing property) for sealing the peripheral portion, a moisture permeation resistance function, and the like, and is made of a moisture permeable hot melt resin containing a desiccant provided on the inner peripheral side of the rubber spacer 4. The sealing material 7 prevents the hollow layer 5 sandwiched between the glass plates 2 and 3 of the multilayer glass 1 from being clouded by moisture.

  FIG. 7 is a partial cross-sectional view of the peripheral edge portion of the multilayer glass 1 according to the sixth embodiment of the present invention. In the multilayer glass 1 of this embodiment, the isobutylene-based polymer (A), the thermoplastic resin (on the periphery of the opposing surface side of at least two glass plates 2 and 3 that are opposed to each other at a predetermined interval ( B) and a rubber spacer 4 containing a compound (C) having a hydrosilyl group are provided, and a sealing material 7 made of a moisture-permeable hot melt resin containing a desiccant is provided on the inner peripheral side of the rubber spacer 4. Further, a resin spacer 6 made of a thermoplastic resin is provided on the outer peripheral side of the rubber spacer 4. The glass spacers 2 and 3 are kept at a predetermined interval by the rubber spacer 4 and the resin spacer 6 so that the hollow layer 5 is formed. Further, the inner peripheral side of the rubber spacer 4 is sealed by the sealing material 7.

  The spacer of this embodiment is composed of a rubber spacer 4, a resin spacer 6, and a sealing material 7. The rubber spacer 4 keeps a space between the glass plates 2 and 3 of the multi-layer glass 1 facing each other. Functions, gas containment (gas barrier property), sealing function (sealing property) for sealing the peripheral portion, moisture permeation resistance function and the like, and the resin spacer 6 is a glass plate 2 facing the multilayer glass 1 3 has a function of maintaining a predetermined distance between the three, and imparts excellent shape maintenance and long-term durability. Furthermore, the sealing material 7 made of a moisture-permeable hot melt resin containing a desiccant provided on the inner peripheral side of the rubber spacer 4 is clouded by moisture in the hollow layer 5 sandwiched between the glass plates 2 and 3 of the multilayer glass 1. To prevent that.

  FIG. 8 is a partial cross-sectional view of the peripheral edge portion of the multilayer glass 1 according to the seventh embodiment of the present invention. In the multilayer glass 1 of this embodiment, the isobutylene-based polymer (A), the thermoplastic resin (on the periphery of the opposing surface side of at least two glass plates 2 and 3 that are opposed to each other at a predetermined interval ( B) and a rubber spacer 4 containing a compound (C) having a hydrosilyl group are provided, a resin spacer 6 made of a thermoplastic resin is provided on the inner peripheral side of the rubber spacer 4, and the resin spacer 6 A sealing material 7 made of a moisture-permeable hot melt resin containing a desiccant is provided on the inner peripheral side. The glass spacers 2 and 3 are kept at a predetermined interval by the rubber spacer 4 and the resin spacer 6 so that the hollow layer 5 is formed. Further, the inner peripheral side of the resin spacer 6 is sealed by the sealing material 7.

  The spacer of this embodiment is composed of a rubber spacer 4, a resin spacer 6, and a sealing material 7. The rubber spacer 4 keeps a space between the glass plates 2 and 3 of the multi-layer glass 1 facing each other. Functions, gas containment (gas barrier property), sealing function (sealing property) for sealing the peripheral portion, moisture permeation resistance function and the like, and the resin spacer 6 is a glass plate 2 facing the multilayer glass 1 3 has a function of maintaining a predetermined distance between the three, and imparts excellent shape maintenance and long-term durability. Further, a sealing material 7 made of a moisture-permeable hot melt resin containing a desiccant provided on the inner peripheral side of the resin spacer 6 is clouded by moisture in the hollow layer 5 sandwiched between the glass plates 2 and 3 of the multilayer glass 1. To prevent that.

  The glass plate used in the multilayer glass of the present invention is not particularly limited, and as such a glass plate, glass plates such as windows and doors that are usually widely used in building materials, vehicles, etc., tempered glass, and laminated glass Glass plates with metal mesh, heat-absorbing glass, glass plates with thin metal or other inorganic coatings on the inner surface, such as heat-reflecting glass and low-reflectance glass, acrylic resin plates called organic glass, polycarbonate plates Etc. Further, the multilayer glass may be composed of two glass plates or may be composed of three or more glass plates.

  Although there is no restriction | limiting in particular regarding the manufacturing method of the multilayer glass of this invention, For example, the said isobutylene type polymer (A) which comprises a rubber-like spacer, a thermoplastic resin (B), and the compound (C) which has a hydrosilyl group In succession to the molding operation of forming a hot melt adhesive resin composition containing a predetermined shape, the obtained molded product is placed at the end of the multi-layer glass material in which two or more glass plates are arranged to face each other. Provide a rubber spacer. Under the present circumstances, the high adhesiveness (hot-melt adhesiveness) with a glass plate is obtained by using the high temperature composition extracted from the molding machine. Moreover, you may provide a rubber-like spacer in a glass plate, suppressing apparatus temperature fall using apparatuses, such as an applicator. This device is preferably a heatable device. If necessary, an adhesive or primer dissolved in a solvent is applied to the glass surface on which the rubber spacer is provided and air-dried, and a general-purpose extruder having a cylinder with an appropriate diameter is used, and the resin composition is For example, it can be formed by melting at a temperature of 80 to 200 ° C. and interposing between two glass plates and cooling while extruding from a die having an appropriate tip shape. Furthermore, as a method for producing the multilayer glass 1 of the first embodiment as described above, a hot containing the isobutylene polymer (A), the thermoplastic resin (B) and the compound (C) having a hydrosilyl group is used. A rubber spacer 4 is extruded into a predetermined spacer shape on the inner surface of the peripheral edge of one of the pair of glass plates 2 and 3 from the resin composition having melt adhesiveness, and the rubber spacer 4 is molded. The other glass plate is pressure-bonded to the glass plate, and the glass spacers 2 and 3 are provided with rubber spacers provided at the peripheral portions of the glass plates 2 and 3 so that the hollow layer 5 is formed between them. 4 in a state of being opposed to each other at a predetermined interval. In addition, the rubber spacer 4 is provided with a sealing material 7 made of a moisture-permeable hot melt resin containing a resin spacer 6 and / or a desiccant on the inner and / or outer peripheral side of the second to seventh embodiments. In the laminated glass, the resin constituting the resin spacer 6 and / or the sealing material 7 is simultaneously extruded (multicolor simultaneous molding) at the time of extrusion molding of the rubber spacer 4, thereby enabling the first embodiment. Multi-layer glass can be produced in the same manner as described above.

  The multi-layer glass 1 of the first embodiment is a resin composition having hot-melt adhesiveness containing the isobutylene polymer (A), the thermoplastic resin (B), and the compound (C) having a hydrosilyl group. The rubber spacer 4 having a predetermined shape is molded in advance, and the rubber spacer 4 is bonded onto the inner surface of one of the peripheral portions of the pair of glass plates 2 and 3 constituting the multilayer glass 1. Another glass plate is pressure-bonded to the glass plate to which the rubber spacer 4 is bonded, and both glass plates 2 and 3 are provided at the peripheral edge of the glass plate so that a hollow layer 5 is formed between them. Further, it can be manufactured by binding in a state of being opposed to each other at a predetermined interval through the rubber spacer 4. Further, the multilayer glass 1 according to the second to seventh embodiments simultaneously extrudes the resin spacer 6 and / or the resin constituting the sealing material 7 at the time of extrusion molding of the rubber spacer 4 (multicolor simultaneous). By molding, a multilayer glass can be produced as in the first embodiment. The rubber spacer 4 can be molded using a molding method and a molding apparatus generally employed for the thermoplastic resin composition, and can be molded by, for example, extrusion molding, injection molding, press molding, blow molding, or the like.

  The rubber spacer 4, the resin spacer 6, and the sealing material 7 as described above may be provided for each side of the peripheral portion of the glass plate 2 (3) as shown in FIG. As shown in FIG. 15, it may be provided continuously over the entire peripheral edge of the glass plate 2 (3) (only the rubber spacer 4 is shown in FIGS. 15 and 16). In any case, at least one joint 10 is formed on the rubber spacer 4 (and also the resin spacer 6 and the sealing material 7) at the peripheral edge of the glass plate 2 (3). The seam 10 is bonded to some extent during hot melting, but there is a possibility that a gap may be formed between the spacers that abut. When a gap is formed in the joint 10 as described above, the gas barrier property is impaired. Therefore, for example, as shown in FIG. 17, a synthetic resin or metal connecting piece 11 is driven between the rubber spacers 4 that are in contact with each other with the joint 10 interposed therebetween. Alternatively, as shown in FIG. The cross section of the sealing piece 12a that extends between the rubber spacers 4 that are in contact with each other across the joint 10 and the insertion piece 12b that protrudes in the direction perpendicular to the sealing piece 12a on the inner surface side of the sealing piece 12a. The T-shaped sealing member 12 is inserted into the seam 10 from the outer peripheral side of the rubber spacer 4, and the outer peripheral side of the seam 10 is sealed with the sealing piece 12a. Gas barrier properties can also be secured. Further, in the case of the rubber spacer 4 (in addition, the resin spacer 6 and the seal material 7) molded in advance, for example, as shown in FIG. 19A, the length of the outer periphery of the glass plate 2 (3) is set. As shown in FIG. 19 (b), an engagement structure composed of a convex portion 4a and a concave portion 4b that are fitted to each other is formed on each of both end portions of the rubber spacer 4 molded to a corresponding length. By connecting both end portions of the rubber spacer 4 in a state where the convex portion 4a and the concave portion 4b are fitted, gas barrier properties at the joint can be ensured. At this time, when the rubber spacer 4 is formed by extrusion, as shown in FIG. 19C, the rubber spacer 4 extruded from the die 13 of the extruder is replaced with the convex portion 4a and the concave portion 4b. The convex portions 4a and the concave portions 4b can be simultaneously formed on both end portions of the rubber spacer 4 by cutting into the shape of The engagement structure at both ends of the rubber spacer 4 is not limited to the fitting structure between the convex part 4a and the concave part 4b as described above. For example, as shown in FIGS. 19 (d) and 19 (e). Such shapes and structures may be used. In the case of the engagement structure shown in FIGS. 19 (d) and 19 (e), the rubber spacer 4 extruded from the die 13 of the extruder is cut into a predetermined shape in the same manner as described above. The engaging structure at both ends of the quality spacer 4 can be formed simultaneously.

  Next, what is shown in FIG. 9 is a partial cross-sectional view of the peripheral edge portion of the multilayer glass 1 according to the eighth embodiment of the present invention. In the multilayer glass 1 of the eighth embodiment, as in the multilayer glass 1 of the sixth embodiment shown in FIG. 7, at least two glass plates 2 and 3 opposed to each other at a predetermined interval are opposed to each other. A rubber spacer 4 containing the isobutylene polymer (A), the thermoplastic resin (B), and a compound having a hydrosilyl group (C) is provided on the peripheral edge of the surface side, and the inner peripheral side of the rubber spacer 4 Further, a sealing material 7 made of a moisture-permeable hot melt resin containing a desiccant is provided, and a resin spacer 6 made of a thermoplastic resin is provided on the outer peripheral side of the rubber spacer 4. The glass plates 2 and 3 are kept at a predetermined interval by the rubber spacer 4 and the resin spacer 6 to form a hollow layer 5, and the inner peripheral side of the rubber spacer 4 is sealed by the sealing material 7. In the multilayer glass 1 of the eighth embodiment, the resin spacer 6 provided on the outermost periphery is formed so as to cover the outer peripheral edges of the glass plates 2 and 3.

  The spacer of this embodiment is composed of a rubber spacer 4, a resin spacer 6, and a sealing material 7. The rubber spacer 4 keeps a space between the glass plates 2 and 3 of the multi-layer glass 1 facing each other. Functions, gas containment (gas barrier property), sealing function (sealing property) for sealing the peripheral portion, moisture permeation resistance function, and the like, and the resin spacer 6 is a glass plate 2 facing the multi-layer glass 1, It has a function of maintaining a predetermined distance between 3 and imparts excellent shape maintenance and long-term durability. Further, the sealing material 7 made of a moisture-permeable hot melt resin containing a desiccant provided on the inner peripheral side of the rubber spacer 4 has a hollow layer 5 sandwiched between the glass plates 2 and 3 of the multilayer glass 1 by moisture. Prevent fogging. Furthermore, the resin spacer 6 protects the outer peripheral edges of the glass plates 2 and 3 and prevents breakage.

  Moreover, what is shown in FIG. 10 is the fragmentary sectional view of the peripheral part of the multilayer glass 1 of 9th Embodiment in this invention. In the multilayer glass 1 of the ninth embodiment, the resin spacer 6 formed on the outermost periphery so as to cover the outer peripheral edges of the glass plates 2 and 3 in the multilayer glass 1 of the eighth embodiment shown in FIG. However, it is made to protrude on the outer surface side of the glass plates 2 and 3.

  The spacer of this embodiment is composed of a rubber spacer 4, a resin spacer 6, and a sealing material 7. The rubber spacer 4 keeps a space between the glass plates 2 and 3 of the multi-layer glass 1 facing each other. Function, gas containment (gas barrier property), sealing function (sealing property) for sealing the peripheral portion, moisture permeation resistance function, and the like, and the resin spacer 6 is a glass plate 2 facing the multi-layer glass 1, It has a function of maintaining a predetermined distance between 3 and imparts excellent shape maintenance and long-term durability. Furthermore, the sealing material 7 made of a moisture-permeable hot melt resin containing a desiccant provided on the inner peripheral side of the rubber spacer 4 is clouded by moisture in the hollow layer 5 sandwiched between the glass plates 2 and 3 of the multilayer glass 1. To prevent that. Further, the outer peripheral edges of the glass plates 2 and 3 are protected by the resin spacer 6 to prevent breakage. Furthermore, the resin spacer 6 protruding to the outer surface side of the glass plates 2 and 3 can also be used as a frame when the multilayer glass 1 is mounted on a sash or the like. The shape of the resin spacer 6 protruding to the outer surface side of the glass plates 2 and 3 is not particularly limited, and can be formed into an arbitrary shape depending on the shape and structure of a sash to be mounted.

  Furthermore, what is shown in FIG. 11 is a partial cross-sectional view of the peripheral edge portion of the multilayer glass 1 of the tenth embodiment of the present invention. In the multilayer glass 1 of this embodiment, the isobutylene-based polymer (A), the thermoplastic resin (on the periphery of the opposing surface side of at least two glass plates 2 and 3 that are opposed to each other at a predetermined interval ( A rubber spacer 4 containing B) and a compound (C) having a hydrosilyl group is provided, and a metal spacer 8 made of, for example, aluminum is provided on the inner peripheral side of the rubber spacer 4. By the rubber spacer 4 and the metal spacer 8, the glass plates 2 and 3 are kept at a predetermined interval, and the hollow layer 5 is formed. The metal spacer 8 may be one in which a desiccant d is filled as shown in FIG.

  The spacer of this embodiment is composed of a rubber spacer 4 and a metal spacer 8, and the rubber spacer 4 has a function of keeping a predetermined distance between the opposing glass plates 2 and 3 of the multi-layer glass 1, and gas containment. (Gas barrier property), sealing function (sealing property) for sealing the peripheral portion, moisture permeation resistance function, and the like, and the metal spacer 8 has a function of keeping the glass plates 2 and 3 at a predetermined interval. Furthermore, excellent shape maintaining property and long-term durability are imparted, and large-sized multilayer glass can be produced.

  The embodiment in which the metal spacer 8 is used in combination is not particularly limited. For example, as shown in FIG. 12, the metal spacer 8 is provided on the outer peripheral side of the rubber spacer 4 (11th embodiment), FIG. As shown in FIG. 4, a metal spacer 8 is provided on the inner peripheral side of the rubber spacer 4, and a sealing material 7 made of a moisture-permeable hot melt resin containing a desiccant is provided on the inner peripheral side (Twelfth Embodiment). ), Or as shown in FIG. 14, a metal spacer 8 is provided on the outer peripheral side of the rubber spacer 4, while a sealing material made of a moisture-permeable hot melt resin containing a desiccant is provided on the inner peripheral side of the rubber spacer 4. Arbitrary combinations, such as providing 7 (13th Embodiment), are possible. Further, the metal spacer 8 does not necessarily have a gap maintaining function, and the thickness (in a direction parallel to the glass plates 2 and 3) is provided for the purpose of giving the multi-layer glass 1 a higher gas barrier property. A thin metal spacer (seal material) may be provided.

  A spacer combining the rubber spacer 4 and the metal spacer 8 as described above, and a spacer combining the rubber spacer 4, the sealing material 7 made of moisture-permeable hot melt resin, and the metal spacer 8 are rubber spacers. When the resin composition is molded, the metal spacer 8 can be inserted in advance and molded by press formation or the like.

  The multilayer glass 1 according to the present invention is not limited to the first to thirteenth embodiments described above, and various spacers such as a rubber spacer 4, a resin spacer 6, a metal spacer 8, and a desiccant. The sealing material 7 made of a moisture-permeable hot melt resin containing can be appropriately combined. Moreover, the thickness (direction parallel to the glass plates 2 and 3) of various spacers such as the rubber spacer 4, the resin spacer 6, and the metal spacer 8 and the seal material 7 is not particularly limited. As long as the object can be achieved, the thicknesses of the various spacers and the sealing material can be set as appropriate.

  In the multi-layer glass according to the present invention configured as described above, the rubber spacer 4 functions to keep the high glass plates 2 and 3 at a predetermined interval, gas containment (gas barrier property), and seal the peripheral portion. Sealing function (sealability) and moisture permeation-proof function are given, and the function of maintaining a predetermined distance between the high glass plates 2 and 3 by the resin spacer 6 and the metal spacer 8, shape maintenance, and long-term The hollow layer 5 sandwiched between the glass plates 2 and 3 of the multi-layer glass 1 by a sealing material 7 made of moisture-permeable hot melt resin containing a desiccant provided on the innermost peripheral side of the spacer. Is prevented from being clouded by moisture. Further, the innermost spacer or sealing material containing a desiccant is effective for removing the initial moisture contained in the hollow layer 5 during the production of the multi-layer glass 1 (initial dew point). The multi-layer glass thus produced is excellent in gas barrier properties, shape maintenance, long-term durability, etc. required as multi-layer glass, and can simplify the manufacturing process.

  Below, the detail is demonstrated about the spacer used for the multilayer glass which concerns on this invention, and a sealing material.

  First, the isobutylene polymer (A) used for the rubber spacer 4 will be described. The isobutylene polymer (A) in the present invention has an alkenyl group at the terminal. The isobutylene polymer (A) having an alkenyl group at the terminal in the present invention means a polymer containing 50% by weight or more of isobutylene based on the total amount of the isobutylene polymer (A). The content of isobutylene is preferably 70% by weight or more, and more preferably 90% by weight or more.

  The monomer other than isobutylene in the isobutylene polymer (A) is not particularly limited as long as it is a monomer component capable of cationic polymerization, but aromatic vinyls, aliphatic olefins, dienes, vinyl ethers, Examples thereof include monomers such as β-pinene. These may be used alone or in combination of two or more.

  Aromatic vinyls include styrene, o-, m- or p-methylstyrene, α-methylstyrene, β-methylstyrene, 2,6-dimethylstyrene, 2,4-dimethylstyrene, α-methyl-o-. Methyl styrene, α-methyl-m-methyl styrene, α-methyl-p-methyl styrene, β-methyl-o-methyl styrene, β-methyl-m-methyl styrene, β-methyl-p-methyl styrene, 2, 4,6-trimethylstyrene, α-methyl-2,6-dimethylstyrene, α-methyl-2,4-dimethylstyrene, β-methyl-2,6-dimethylstyrene, β-methyl-2,4-dimethylstyrene , O-, m- or p-chlorostyrene, 2,6-dichlorostyrene, 2,4-dichlorostyrene, α-chloro-o-chlorostyrene, α-chloro-m-alkyl Rollostyrene, α-chloro-p-chlorostyrene, β-chloro-o-chlorostyrene, β-chloro-m-chlorostyrene, β-chloro-p-chlorostyrene, 2,4,6-trichlorostyrene, α-chloro -2,6-dichlorostyrene, α-chloro-2,4-dichlorostyrene, β-chloro-2,6-dichlorostyrene, β-chloro-2,4-dichlorostyrene, o-, m- or pt -Butyl styrene, o-, m- or p-methoxy styrene, o-, m- or p-chloromethyl styrene, o-, m- or p-bromomethyl styrene, styrene derivatives substituted with silyl groups, indene, Examples include vinyl naphthalene. These may be used alone or in combination of two or more.

  Aliphatic olefins include ethylene, propylene, 1-butene, 2-methyl-1-butene, 3-methyl-1-butene, pentene, hexene, cyclohexene, 4-methyl-1-pentene, vinylcyclohexane, octene, Examples include norbornene. These may be used alone or in combination of two or more.

  Examples of dienes include butadiene, isoprene, hexadiene, cyclopentadiene, cyclohexadiene, dicyclopentadiene, divinylbenzene, and ethylidene norbornene. These may be used alone or in combination of two or more.

  Examples of vinyl ethers include methyl vinyl ether, ethyl vinyl ether, (n-, iso) propyl vinyl ether, (n-, sec-, tert-, iso) butyl vinyl ether, methyl propenyl ether, ethyl propenyl ether and the like. These may be used alone or in combination of two or more.

  Although there is no restriction | limiting in particular in the molecular weight of an isobutylene type polymer (A), 1,000-500,000 are preferable at a number average molecular weight, and 5,000-200,000 are especially preferable. When the number average molecular weight is less than 1,000, there is a tendency that the adhesiveness at the time of hot melt adhesion is not sufficiently exhibited. Moreover, when it exceeds 500,000, there exists a tendency for the fluidity | liquidity at the time of hot-melt adhesion to fall. The number average molecular weight in the present specification is a value measured by gel permeation chromatography and expressed in terms of polystyrene.

  The isobutylene polymer (A) can be produced by isobutylene alone or by cationic polymerization of isobutylene and another monomer.

  The alkenyl group in the present invention is not particularly limited as long as it is a group containing a carbon-carbon double bond active for the hydrosilylation reaction of the component (A) for achieving the object of the present invention. Absent. Specific examples include aliphatic unsaturated hydrocarbon groups such as vinyl group, allyl group, methyl vinyl group, propenyl group, butenyl group, pentenyl group, hexenyl group, cyclopropenyl group, cyclobutenyl group, cyclopentenyl group, cyclohexenyl group. And cyclic unsaturated hydrocarbon groups such as

  The isobutylene polymer (A) has a functional group such as a hydroxyl group as disclosed in JP-A-3-152164 and JP-A-7-304909 as a method for introducing an alkenyl group at the terminal. Examples thereof include a method of introducing an unsaturated group into a polymer by reacting a compound having an unsaturated group with the polymer. In order to introduce an unsaturated group into a polymer having a halogen atom, a method of performing a Friedel-Crafts reaction with an alkenylphenyl ether, a method of performing a substitution reaction with allyltrimethylsilane in the presence of a Lewis acid, Examples include a method in which a Friedel-Crafts reaction with a phenol is performed to introduce a hydroxyl group, and then the alkenyl group introduction reaction is further performed. Further, as disclosed in U.S. Pat. No. 4,316,973, JP-A-63-105005, and JP-A-4-288309, it is possible to introduce an unsaturated group during polymerization of the monomer. . Among these, a method of introducing an allyl group at the terminal by a substitution reaction between allyltrimethylsilane and chlorine at the terminal of the isobutylene polymer is preferable from the viewpoint of introduction reliability.

  The amount of terminal alkenyl groups of the isobutylene polymer (A) is preferably a polymer having at least 0.2 alkenyl groups per molecule per molecule, and a polymer having at least one alkenyl group at the end. More preferably, it is a coalescence. If it is less than 0.2, the reaction with the compound (C) described later becomes insufficient, and the melt viscosity at high temperature decreases. As a result, the shape may not be maintained when bonded to a substrate such as glass by hot melt.

  The content of the isobutylene polymer (A) in the resin composition constituting the rubber spacer 4 varies depending on the various components used together and cannot be specified unconditionally, but it is preferably 10% by weight or more, preferably 20% by weight or more. Is more preferable. Below this value, the gas barrier properties tend to deteriorate.

  Next, the thermoplastic resin (B) is not particularly limited, but for example, at least one selected from the group consisting of plastics, rubbers, and thermoplastic elastomers can be used.

  Examples of the plastics include polyolefins such as polypropylene and polyethylene, polystyrene, ABS, MBS, acrylic, polyurethane, polyvinyl chloride, polyester, polyamide, and the like. Of these, polyethylene, polypropylene, and polyethylene-α-olefin copolymers that flow at lower temperatures and have high gas barrier properties are preferred. Examples of the polyethylene-α olefin copolymer include ethylene-propylene copolymer, ethylene-butene copolymer, ethylene-hexene copolymer, ethylene-octene copolymer, ethylene-vinyl acetate copolymer, ethylene-acrylic acid. Examples include ethyl copolymers.

  Examples of rubbers include polyether, polybutadiene, natural rubber, polyisobutylene, isobutylene-isoprene copolymer (butyl rubber), chlorinated butyl, brominated butyl, isobutylene- (p-methylstyrene) copolymer, isobutylene- Examples thereof include brominated products of (p-methylstyrene) copolymer, chloroprene rubber, and ethylene-propylene rubber. Of these, polyisobutylene, isobutylene-isoprene copolymer (butyl rubber), chlorinated butyl, brominated butyl, isobutylene- (p-methylstyrene) copolymer, brominated product of isobutylene- (p-methylstyrene) copolymer Is preferable from the viewpoint of gas barrier properties.

  Examples of the thermoplastic elastomer include, for example, a styrene-based thermoplastic elastomer that is a block copolymer composed of a polystyrene block and a polybutadiene or polyisoprene block, an olefin-based composed of a polyolefin component such as polypropylene and a rubber component such as ethylene-propylene rubber. Thermoplastic elastomers, vinyl chloride thermoplastic elastomers composed of crystalline and amorphous polyvinyl chloride, urethane thermoplastic elastomers that are block copolymers composed of polyurethane blocks and polyether blocks, polyester blocks and polyether blocks, etc. Polyester-based thermoplastic elastomer, which is a block copolymer comprising amide, and amide-based thermoplastic, which is a block copolymer comprising a polyamide block and a polyether block Elastomers, and the like. Of these thermoplastic elastomers, styrene-based thermoplastic elastomers and urethane-based thermoplastic elastomers are particularly preferable in terms of softening point and hot-melt adhesiveness with the glass surface. These may be used alone or in combination of two or more.

  Although there is no restriction | limiting as a styrene-type thermoplastic elastomer, For example, the conjugated diene type block copolymer which consists of a polymer block which uses an aromatic vinyl compound as a constituent monomer, and a polymer block which contains a conjugated diene as a constituent monomer A hydrogenated conjugated diene block copolymer comprising a polymer block comprising an aromatic vinyl compound as a constituent monomer and a polymer block comprising a hydrogenated conjugated diene as a constituent monomer, and an aromatic vinyl compound comprising An isobutylene block copolymer (hereinafter referred to as “isobutylene block copolymer (B1)”) comprising a polymer block (a) as a monomer and a polymer block (b) having isobutylene as a constituent monomer. In particular, from the viewpoint of gas barrier properties, the isobutylene block copolymer (B1) is most preferable.

  Examples of the polymer block having a conjugated diene as a constituent monomer include a polybutadiene block, a polyisoprene block, and a block composed of a combination of butadiene and isoprene. Examples of the polymer block having a hydrogenated conjugated diene as a structural unit include a partially hydrogenated conjugated diene polymer block and a fully hydrogenated conjugated diene polymer block (for example, an ethylene-butylene copolymer). Block, ethylene-propylene copolymer block) and the like. Examples of the aromatic vinyl compound include those composed of at least one monomer selected from the group consisting of styrene, α-methylstyrene, p-methylstyrene, and indene. From the viewpoint of cost, styrene, α -Methylstyrene or mixtures thereof are preferred.

  The isobutylene block copolymer (B1) is not particularly limited, but a polymer block (a) containing an aromatic vinyl compound as a constituent monomer and a polymer block (b) containing isobutylene as a constituent monomer. It is preferable in terms of hot melt workability and molecular weight control. The structure is not particularly limited. For example, a block copolymer, a diblock copolymer, a triblock copolymer, a multiblock copolymer, etc. having a linear, branched, or star structure. Either can be selected. A preferred block copolymer is a polymer block (a) having an aromatic vinyl compound as a constituent monomer and a polymer block (b) having an isobutylene as a constituent monomer from the viewpoint of balance of physical properties. A triblock copolymer comprising a polymer block (a) having a compound as a constituent monomer, and a polymer block (a) -isobutylene having a constituent monomer as an aromatic vinyl compound. A diblock copolymer comprising a block (b), a polymer block comprising an aromatic vinyl compound as a constituent monomer (a) -three arms comprising a polymer block (b) comprising isobutylene as a constituent monomer Examples thereof include the star-shaped block copolymers described above, and triblock copolymers and diblock copolymers are particularly preferable. These can be used alone or in combination of two or more in order to obtain desired physical properties and hot melt processability.

  The aromatic vinyl compound constituting the polymer block (a) is not particularly limited, but a compound having an aromatic ring and a cation-polymerizable carbon-carbon double bond can be combined with the polymer block (b). It is preferable at the point which manufactures a polymer. Examples of such compounds include styrene, p-methylstyrene, α-methylstyrene, p-chlorostyrene, pt-butylstyrene, p-methoxystyrene, p-chloromethylstyrene, p-bromomethylstyrene, Examples thereof include styrene derivatives substituted with silyl groups, and indene. These may be used alone or in combination of two or more. Among these, at least one selected from the group consisting of styrene, α-methylstyrene, p-methylstyrene and indene is preferable, and styrene, α-methylstyrene, or a mixture thereof is particularly preferable from the viewpoint of cost. .

  The polymer block (a) may or may not contain a monomer other than the aromatic vinyl compound. When a monomer other than the aromatic vinyl compound is included, the aromatic vinyl compound preferably accounts for 60% by weight or more in the entire polymer block (a), and further accounts for 80% by weight or more. preferable. When the aromatic vinyl compound is 60% by weight or less in the entire polymer block (a), the cohesive force of the polymer block (a) decreases, which is not preferable. The monomer other than the aromatic vinyl compound in the polymer block (a) is not particularly limited as long as it is a monomer that can be cationically polymerized with the aromatic vinyl compound, and examples thereof include isobutylene, aliphatic olefins, and dienes. And monomers such as vinyl ethers and β-pinene. These may be used alone or in combination of two or more.

  Although there is no restriction | limiting in particular as a molecular weight of the polymer block (a) which uses an aromatic vinyl compound as a structural monomer, It is preferable that it is 30,000 or less by a number average molecular weight. By satisfying such a number average molecular weight, a material that can be hot-melt processed (that is, has a low melt viscosity when heated to a high temperature) can be obtained. When the number average molecular weight is 30,000 or more, it is difficult to melt even at high temperatures, so that hot melt processing is difficult.

  The number average molecular weight of the polymer block (a) is further preferably 1,000 or more and 20,000 or less. If the number average molecular weight of the polymer block (a) is too low, the fluidity at room temperature increases and the cold flow property is exhibited, which tends to cause a problem with respect to shape maintainability.

  The polymer block (b) constituting the isobutylene block copolymer (B1) in the present invention is a polymer block comprising isobutylene as a constituent monomer.

  Although it does not specifically limit as molecular weight of a polymer block (b), It is preferable to adjust so that the number average molecular weight of the whole isobutylene type block copolymer (B1) may become the preferable value described below.

  The polymer block (b) may or may not contain a monomer other than isobutylene. When a monomer other than isobutylene is included, isobutylene preferably occupies 60% by weight or more, and more preferably 80% by weight or more in the entire polymer block (b). The monomer other than isobutylene in the polymer block (b) is not particularly limited as long as it is a monomer capable of cationic polymerization with isobutylene. For example, the aromatic vinyl compounds, aliphatic olefins, and dienes described above are used. And monomers such as vinyl ethers and β-pinene. These may be used alone or in combination of two or more.

  In the isobutylene block copolymer (B1), the ratio of the polymer block (a) having an aromatic vinyl compound as a constituent monomer and the polymer block (b) having an isobutylene as a constituent monomer is particularly limited. However, from the balance between gas barrier properties and hot melt properties, the weight ratio of polymer block (a): polymer block (b) is preferably 5:95 to 40:60, 10:90 to 40: 60 is more preferable.

  The molecular weight of the isobutylene block copolymer (B1) is not particularly limited, but is preferably 3,000 to 500,000 in terms of number average molecular weight from the viewpoint of hot melt adhesiveness and processability, and 5,000. More preferably, it is ˜300,000. When the number average molecular weight of the isobutylene-based block copolymer (B1) is lower than the above range, the fluidity near room temperature becomes high and easily deforms. The fluidity at the time becomes insufficient and the hot melt workability tends to be inferior.

The production method of the isobutylene block copolymer (B1) is not particularly limited, and a known polymerization method can be used. In order to obtain a block copolymer having a controlled structure, the following general formula ( In the presence of the compound represented by 1), it is preferable to polymerize a monomer component mainly composed of isobutylene and a monomer component mainly composed of an aromatic vinyl compound.
(CR ¹ R ² X) nR ³ (1)
[Wherein, X represents a substituent selected from the group consisting of a halogen atom, an alkoxyl group having 1 to 6 carbon atoms and an acyloxyl group having 1 to 6 carbon atoms. R ¹ , R ² and R ³ are each a hydrogen atom, an aliphatic hydrocarbon group or an aromatic hydrocarbon group, and R ¹ , R ² and R ³ may be the same or different. n shows the natural number of 1-6. ]

  Examples of the halogen atom include chlorine, fluorine, bromine, iodine and the like. It does not specifically limit as said C1-C6 alkoxyl group, For example, a methoxy group, an ethoxy group, n- or an isopropoxy group etc. are mentioned. It does not specifically limit as said C1-C6 acyloxyl group, For example, an acetyloxy group, a propionyloxy group, etc. are mentioned. The aliphatic hydrocarbon group is not particularly limited, and examples thereof include a methyl group, an ethyl group, an n- or isopropyl group. The aromatic hydrocarbon group is not particularly limited, and examples thereof include a phenyl group and a methylphenyl group.

  The compound represented by the general formula (1) serves as an initiator, and is considered to generate a carbon cation in the presence of a Lewis acid or the like and serve as a starting point for cationic polymerization. Examples of the compound of the general formula (1) used in the present invention include the following compounds.

(1-Chloro-1-methylethyl) benzene [C ₆ H ₅ C (CH ₃ ) ₂ Cl], 1,4-bis (1-chloro-1-methylethyl) benzene [1,4-Cl (CH ₃ ) ₂ CC ₆ H ₄ C (CH ₃ ) ₂ Cl], 1,3-bis (1-chloro-1-methylethyl) benzene [1,3-Cl (CH ₃ ) ₂ CC ₆ H ₄ C (CH ₃ ) ₂ Cl], 1,3,5-tris (1-chloro-1-methylethyl) benzene [1,3,5- (ClC (CH ₃ ) ₂ ) ₃ C ₆ H ₃ ], 1,3-bis (1-Chloro-1-methylethyl) -5- (tert-butyl) benzene [1,3- (C (CH ₃ ) ₂ Cl) ₂ -5 (C (CH ₃ ) ₃ ) C ₆ H ₃ ]
Among these, (1-chloro-1-methylethyl) benzene [C ₆ H ₅ C (CH ₃ ) ₂ Cl], bis (1-chloro-1-methylethyl) benzene [C ₆ H ₄ is particularly preferable. (C (CH ₃ ) ₂ Cl) ₂ ], tris (1-chloro-1-methylethyl) benzene [(ClC (CH ₃ ) ₂ ) ₃ C ₆ H ₃ ]. [(1-Chloro-1-methylethyl) benzene is also called (α-chloroisopropyl) benzene, (2-chloro-2-propyl) benzene or cumyl chloride, and is bis (1-chloro-1-methyl). Ethyl) benzene is also called bis (α-chloroisopropyl) benzene, bis (2-chloro-2-propyl) benzene or dicumyl chloride, and tris (1-chloro-1-methylethyl) benzene is tris (α -Also called chloroisopropyl) benzene, tris (2-chloro-2-propyl) benzene or tricumyl chloride].

When the isobutylene block copolymer (B1) is produced by polymerization, a Lewis acid catalyst can be allowed to coexist. Such Lewis acid may be any one that can be used for cationic polymerization. TiCl ₄ , TiBr ₄ , BCl ₃ , BF ₃ , BF ₃ .OEt ₂ , SnCl ₄ , SbCl ₅ , SbF ₅ , WCl ₆ , TaCl ₅ , VCl ₅ , FeCl ₃ , ZnBr ₂ , AlCl ₃ , AlBr _3, etc .; metal halides such as Et ₂ AlCl, EtAlCl _2, etc. can be preferably used. Of these, TiCl ₄ , BCl ₃ , and SnCl ₄ are preferable in view of the ability as a catalyst and industrial availability. The amount of Lewis acid used is not particularly limited, but can be set in view of the polymerization characteristics or polymerization concentration of the monomer used. Usually, it is 0.1-100 mol equivalent with respect to the compound represented by General formula (1), Preferably it is the range of 1-50 mol equivalent.

  In the polymerization of the isobutylene block copolymer (B1), an electron donor component can be further present if necessary. This electron donor component is considered to have an effect of stabilizing the growth carbon cation during cationic polymerization, and a polymer having a controlled structure with a narrow molecular weight distribution is formed by addition of the electron donor. The electron donor component that can be used is not particularly limited, and examples thereof include pyridines, amines, amides, sulfoxides, esters, and metal compounds having an oxygen atom bonded to a metal atom.

  The polymerization of the isobutylene-based block copolymer (B1) can be carried out in an organic solvent as necessary, and the organic solvent can be used without particular limitation as long as it does not substantially inhibit cationic polymerization. Specifically, halogenated hydrocarbons such as methyl chloride, dichloromethane, chloroform, ethyl chloride, dichloroethane, n-propyl chloride, n-butyl chloride, chlorobenzene; benzene, toluene, xylene, ethylbenzene, propylbenzene, butylbenzene, etc. Alkylbenzenes; linear aliphatic hydrocarbons such as ethane, propane, butane, pentane, hexane, heptane, octane, nonane, decane; 2-methylpropane, 2-methylbutane, 2,3,3-trimethylpentane, 2 Branched aliphatic hydrocarbons such as 1,2,5-trimethylhexane; cycloaliphatic hydrocarbons such as cyclohexane, methylcyclohexane and ethylcyclohexane; paraffin oil obtained by hydrorefining petroleum fractions, etc. .

  These solvents are used singly or in combination of two or more in consideration of the balance of the polymerization characteristics of the monomers constituting the isobutylene block copolymer (B1) and the solubility of the resulting polymer. The amount of the solvent used is determined so that the concentration of the polymer is 1 to 50 wt%, preferably 5 to 35 wt%, in consideration of the viscosity of the resulting polymer solution and the ease of heat removal.

  In carrying out the actual polymerization, the respective components are mixed under cooling, for example, at a temperature of −100 ° C. or higher and lower than 0 ° C. In order to balance the energy cost and the stability of polymerization, a particularly preferred temperature range is −30 ° C. to −80 ° C. The polymerization reaction may be performed in a batch system (batch system or semi-batch system), or may be performed in a continuous system in which each component necessary for the polymerization reaction is continuously added to the polymerization vessel.

  Moreover, what has various functional groups in a molecular chain or a molecular chain terminal can be used as a thermoplastic resin (B) for the objective, such as improving the adhesiveness to the glass plate of the composition of this invention. Examples of the functional group include an ether group such as an epoxy group, a hydroxyl group, an amino group, an alkylamino group, and an alkoxyl group, an ester group such as a carboxyl group, an alkoxycarbonyl group, and an acyloxy group, a carbamoyl group, an alkylcarbamoyl group, and an acylamino group. Amide groups, acid anhydride groups such as maleic anhydride, silyl groups, allyl groups, vinyl groups, and the like. The thermoplastic resin (B) may have only one type of these functional groups, or may have two or more types.

  These thermoplastic resins (B) can be used alone or in combination of two or more, regardless of the types of plastics, rubbers, and thermoplastic elastomers. The amount is preferably 1 to 300 parts by weight, more preferably 10 to 200 parts by weight, based on 100 parts by weight of the combined body (A).

  Compound (C) is a compound having at least two hydrosilyl groups in the molecule. Here, having at least two hydrosilyl groups in a molecule means that two or more hydrosilyl groups are contained on average in one molecule. When two hydrogen atoms are bonded to the same silicon atom, it is calculated as two silicon atom-bonded hydrogen atoms (hydrosilyl groups).

  These hydrosilyl groups are chemically bonded to the compound (D) having a terminal alkenyl group and / or a carbon-carbon unsaturated bondable functional group described later by a hydrosilylation reaction of the isobutylene polymer (A). It is desirable. In particular, one hydrosilyl group is bonded to the terminal alkenyl group of the isobutylene polymer (A), and the other hydrosilyl group is bonded to the compound (D) having a carbon-carbon unsaturated bondable functional group described later. It is desirable that By bonding in this manner, the composition has sufficient adhesion durability.

  As the compound (C) having at least two hydrosilyl groups in the molecule, polyorganohydrogensiloxane (C1) containing at least two or more hydrosilyl groups in one molecule on average is mentioned as one of preferable ones. It is done. The polyorganohydrogensiloxane (C1) preferably has a siloxane unit in the range of 2 to 500, more preferably 2 to 200. When the number of siloxane units exceeds 500, the viscosity of the polysiloxane is high, the dispersion into the isobutylene polymer (A) becomes insufficient, and the reaction tends to be uneven.

Examples of the siloxane unit in the present invention include the following general formulas (2) to (4). Among these, general formula (3) has a hydrosilyl group.
[Si (R ¹ ) ₂ O] (2)
[Si (H) (R ² ) O] (3)
[Si (R ² ) (R ³ ) O] (4)
As the polyorganohydrogensiloxane (C1) having two or more hydrosilyl groups and two or more and 500 or less siloxane units, a linear polysiloxane represented by the following general formula (5) or (6);

（式中、Ｒ¹およびＲ²はそれぞれ独立して、炭素数１〜１８のアルキル基、炭素数６〜１８のアリール基、炭素数１〜１８のハロゲン化アルキル基、炭素数６〜１８のハロゲン化アリール基、炭素数１〜６のアルコキシ基、炭素数６〜１０のアリーロキシ基、塩素原子を、Ｒ³は炭素数１〜１８のアルキル基、炭素数６〜１８のアリール基、炭素数１〜１８のハロゲン化アルキル基、炭素数６〜１８のハロゲン化アリール基、炭素数１〜６のアルコキシ基、炭素数６〜１０のアリーロキシ基、塩素原子、炭素数７〜１８のアラルキル基、を示す。ａ，ｂ，ｃは、ａ≧０、ｂ≧２、ｃ≧０、２≦ａ＋ｂ＋ｃ≦５００を満たす整数を表す。）等の化合物を用いることができ、また、下記一般式（７）で表される環状ポリシロキサン；

(In the formula, R ¹ and R ² are each independently an alkyl group having 1 to 18 carbon atoms, an aryl group having 6 to 18 carbon atoms, a halogenated alkyl group having 1 to 18 carbon atoms, or an alkyl group having 6 to 18 carbon atoms. A halogenated aryl group, an alkoxy group having 1 to 6 carbon atoms, an aryloxy group having 6 to 10 carbon atoms, and a chlorine atom; R ³ is an alkyl group having 1 to 18 carbon atoms; an aryl group having 6 to 18 carbon atoms; A halogenated alkyl group having 1 to 18 carbon atoms, a halogenated aryl group having 6 to 18 carbon atoms, an alkoxy group having 1 to 6 carbon atoms, an aryloxy group having 6 to 10 carbon atoms, a chlorine atom, an aralkyl group having 7 to 18 carbon atoms, A, b, and c can be compounds such as a ≧ 0, b ≧ 2, c ≧ 0, 2 ≦ a + b + c ≦ 500), and the following general formula (7 ) Cyclic polysiloxane represented by:

（式中、Ｒ¹およびＲ²はそれぞれ独立して、炭素数１〜１８のアルキル基、炭素数６〜１８のアリール基、炭素数１〜１８のハロゲン化アルキル基、炭素数６〜１０のハロゲン化アリール基、炭素数１〜６のアルコキシ基、炭素数６〜１０のアリーロキシ基、塩素原子を、Ｒ³は炭素数１〜１８のアルキル基、炭素数６〜１８のアリール基、炭素数１〜１８のハロゲン化アルキル基、炭素数６〜１８のハロゲン化アリール基、炭素数１〜６のアルコキシ基、炭素数６〜１０のアリーロキシ基、塩素原子、炭素数７〜１８のアラルキル基を示す。ａ，ｂ，ｃは、ａ≧０、ｂ≧２、ｃ≧０、２≦ａ＋ｂ＋ｃ≦５００を満たす整数を表す。）等の化合物を用いることができる。

Wherein R ¹ and R ² are each independently an alkyl group having 1 to 18 carbon atoms, an aryl group having 6 to 18 carbon atoms, a halogenated alkyl group having 1 to 18 carbon atoms, or a 6 to 10 carbon atom. A halogenated aryl group, an alkoxy group having 1 to 6 carbon atoms, an aryloxy group having 6 to 10 carbon atoms, and a chlorine atom; R ³ is an alkyl group having 1 to 18 carbon atoms; an aryl group having 6 to 18 carbon atoms; A halogenated alkyl group having 1 to 18 carbon atoms, a halogenated aryl group having 6 to 18 carbon atoms, an alkoxy group having 1 to 6 carbon atoms, an aryloxy group having 6 to 10 carbon atoms, a chlorine atom, and an aralkyl group having 7 to 18 carbon atoms. A, b, and c are integers satisfying a ≧ 0, b ≧ 2, c ≧ 0, and 2 ≦ a + b + c ≦ 500.

When R ¹ , R ² and R ^{3 in the} general formulas (2) to (7) are alkyl groups having 1 to 18 carbon atoms, for example, methyl group, ethyl group, n-propyl group, isopropyl group, n-butyl group , T-butyl group, n-pentyl group, cyclohexyl group, n-octyl group, nonyl group, undecyl group, heptadecyl group and the like. In the case where R ¹ , R ² and R ^{3 in the} general formulas (2) to (7) are aryl groups having 6 to 18 carbon atoms, for example, phenyl group, p-methylphenyl group, p-methoxyphenyl group and p-tert -A butylphenyl group etc. can be mentioned.

When R ¹ , R ² and R ^{3 in the} general formulas (2) to (7) are halogenated alkyl groups having 1 to 18 carbon atoms, the halogen atom may be F, Cl or Br. Examples thereof include a chloromethyl group, a fluoromethyl group, a 2-chloroethyl group, a 1,1,2,2,2-pentafluoroethyl group, and a 3,3,3-trifluoropropyl group. it can. When R ¹ , R ² and R ^{3 in the} general formulas (2) to (7) are halogenated aryl groups having 6 to 10 carbon atoms, the halogen atom may be F, Cl or Br. -Chlorophenyl group, m-chlorophenyl group, m-chloro-p-methylphenyl group, m-chloro-p-methoxyphenyl group and the like can be mentioned.

When R ¹ , R ² and R ^{3 in the} general formulas (2) to (7) are alkoxy groups having 1 to 6 carbon atoms, for example, methoxy group, ethoxy group, n-propoxy group, i-propoxy group, n- Examples thereof include a butoxy group, an n-pentyloxy group, an n-hexyloxy group, a cyclopentyloxy group, a cyclohexyloxy group, a 2-methoxyethoxy group, and a 2-ethoxyethoxy group. When R ¹ , R ² and R ^{3 in the} general formulas (2) to (7) are aryloxy groups having 6 to 10 carbon atoms, for example, phenoxy group, p-methylphenoxy group, p-methoxyphenoxy group, p-chloro A phenoxy group, m-chlorophenoxy group, etc. can be mentioned.

When R ³ in the general formulas (4) to (7) is an aralkyl group having 7 to 18 carbon atoms, for example, benzyl, phenylethyl, phenylpropyl, 1-phenyl-1-methylethyl, 4-methylphenylethyl, etc. Can be mentioned.

  In the present invention, the compound (C) having at least two hydrosilyl groups in the molecule should have a good compatibility with the isobutylene polymer (A) and the compound (D) or a good dispersion stability in the system. It is preferable to use it, and a plurality of types of compounds (C) can be used in combination. Moreover, the compound (C) may contain components other than the compound which has a hydrosilyl group.

  In order to obtain high rubber elasticity suitable for the sealing material, the compound (C) desirably contains three or more hydrosilyl groups in one molecule. Thereby, the network by bridge | crosslinking will fully grow. As described above, when the crosslinking reaction is efficiently performed using a compound containing three or more hydrosilyl groups in one molecule, the total hydrosilyl group-containing compound (C) contains a compound having at least three hydrosilyl groups. The amount is preferably 10% by weight or more.

  The isobutylene polymer (A) and the compound (C) can be mixed at an arbitrary ratio. From the viewpoint of the hydrosilylation reaction, the alkenyl group of the isobutylene polymer (A) and the hydrosilyl group of the compound (C). The molar ratio of (alkenyl group / hydrosilyl group) is preferably in the range of 0.01 to 10, more preferably 0.03 to 5. When the molar ratio exceeds 10, the hydrosilylation reaction becomes insufficient, and the strength and adhesiveness of the sealing material composition tend to be lowered. Moreover, when it is less than 0.01, many active hydrosilyl groups remain in the composition, and cracks and voids are likely to be generated, and it tends to be difficult to obtain a uniform and strong composition.

  The carbon-carbon unsaturated bond functional group-containing compound (D) is a compound having a hydrosilyl group (C) as in the reaction of the alkenyl group of the isobutylene polymer (A) with the hydrosilyl group of the compound (C). ) And a chemically bonded state is preferable. The compound (D) is not particularly limited as long as it is a compound containing one carbon-carbon double bond having reactivity with a hydrosilyl group in one molecule, but C, H, N, O, S as constituent elements In addition, it preferably contains only halogen, and the bonding position of the carbon-carbon double bond having reactivity with the hydrosilyl group is not particularly limited, and may be present anywhere in the molecule.

  The compound (D) can be classified into a polymer compound and a monomer compound. Examples of the polymer compound include polysiloxane, polyether, polyester, polyarylate, polycarbonate, and saturated hydrocarbons other than polyisobutylene, unsaturated hydrocarbons, polyacrylates, and polyamides. Phenol-formaldehyde (phenolic resin) and polyimide compounds can be used.

  Examples of monomeric compounds include, for example, aromatic hydrocarbons such as phenols, bisphenols, benzene, and naphthalene: aliphatic hydrocarbons such as linear and alicyclics: heterocyclic compounds, and silicons. And a mixture thereof.

  Although it does not specifically limit as a carbon-carbon double bond reactive with the hydrosilyl group of a compound (D), following General formula (8)

（式中Ｒ⁴は水素原子あるいはメチル基を表す。）で示される基が反応性の点から好適である。また、原料の入手の容易さからは、

A group represented by the formula (wherein R ⁴ represents a hydrogen atom or a methyl group) is preferred from the viewpoint of reactivity. In addition, from the availability of raw materials,

で示される基が特に好ましい。

Is particularly preferred.

  As the carbon-carbon double bond having reactivity with the hydrosilyl group of the compound (D), the following general formula (9)

（式中Ｒ⁵は水素原子あるいはメチル基を表す。）で示される脂環式の基が、シール材組成物の耐熱性を向上させ得る点から好適である。また、原料の入手の容易さからは、

An alicyclic group represented by the formula (wherein R ⁵ represents a hydrogen atom or a methyl group) is preferable because it can improve the heat resistance of the sealing material composition. In addition, from the availability of raw materials,

で示される脂環式の基が特に好ましい。

The alicyclic group represented by is particularly preferable.

  The carbon-carbon double bond having reactivity with the hydrosilyl group may be directly bonded to the skeleton portion of the compound (D), or may be covalently bonded via a divalent or higher valent substituent. The divalent or higher valent substituent is not particularly limited as long as it is a substituent having 0 to 10 carbon atoms. However, in terms of easy compatibility with the isobutylene polymer (A), the constituent elements are C and H. , N, O, S, and those containing only halogen are preferred. Examples of these substituents include

が挙げられる。

Is mentioned.

  Specific examples of the compound (D) include propene, 1-butene, 1-pentene, 1-hexene, 1-heptene, 1-octene, 1-nonene, 1-decene, 1-dodecene, 1-undecene, Idemitsu Petrochemical's linearene, 4,4-dimethyl-1-pentene, 2-methyl-1-hexene, 2,3,3-trimethyl-1-butene, 2,4,4-trimethyl-1-pentene, etc. Chain aliphatic hydrocarbon compounds such as cyclohexene, methylcyclohexene, methylenecyclohexane, norbornylene, ethylidenecyclohexane, vinylcyclohexane, camphene, carene, α-pinene, β-pinene and the like, Styrene, α-methylstyrene, indene, phenylacetylene, 4-ethynyltoluene, allylbenzene, 4- Aromatic hydrocarbon compounds such as phenyl-1-butene, allyl ethers such as alkyl allyl ether and allyl phenyl ether, glycerin monoallyl ether, ethylene glycol monoallyl ether, 4-vinyl-1,3-dioxolane- Substitution of aliphatic compounds such as 2-one, aromatic compounds such as 1,2-dimethoxy-4-allylbenzene, o-allylphenol, monoallyl dibenzyl isocyanurate, monoallyl diglycidyl isocyanurate, etc. Examples include isocyanurates, silicon compounds such as vinyltrimethylsilane, vinyltrimethoxysilane, and vinyltriphenylsilane. Furthermore, a vinyl group at one end of a polyether resin such as one end allylated polyethylene oxide, one end allylated polypropylene oxide, one end allylated polybutyl acrylate, one end allylated polymethyl methacrylate, etc. There may also be mentioned polymers or oligomers having

  The structure may be linear or branched, and the molecular weight is not particularly limited, and various types can be used. The molecular weight distribution is not particularly limited, but the molecular weight distribution is preferably 3 or less, more preferably 2 or less, and 1.5 or less in that the viscosity of the mixture tends to be low and the moldability tends to be good. More preferably.

  The compound (D) preferably has a reactive group other than a carbon-carbon double bond. Examples of the reactive group in this case include an epoxy group, an alkoxy group, an amino group, a radical polymerizable unsaturated group, a carboxyl group, a carboxylic anhydride group, an isocyanate group, a hydroxyl group, a halogen atom, and an alkoxysilyl group. . When these functional groups are included, the adhesive property of the resulting sealing material composition tends to be high. Of these functional groups, an epoxy group is preferable from the viewpoint that the adhesiveness can be further increased. Moreover, it is preferable to have at least one reactive group on average in one molecule in that the adhesiveness tends to be high. Specific examples include monoallyl diglycidyl isocyanurate, allyl glycidyl ether, allyloxyethyl methacrylate, allyloxyethyl acrylate, vinyltrimethoxysilane, and the like.

  The above compounds (D) may be used alone or in combination of two or more.

  The compound (D) can be mixed in the composition at an arbitrary ratio. From the viewpoint of the hydrosilylation reaction, the carbon-carbon double bond in the compound (D) and the hydrosilyl group in the compound (C) can be used. The molar ratio (carbon-carbon double bond / hydrosilyl group) is preferably in the range of 0.01 to 10, more preferably 0.02 to 5. When the molar ratio exceeds 10, the hydrosilylation reaction becomes insufficient, and the adhesiveness of the sealing material composition tends to decrease. Moreover, when it is less than 0.01, many active hydrosilyl groups remain in the composition, and cracks and voids are likely to be generated, and it tends to be difficult to obtain a uniform and strong composition.

  Next, the reaction performed between the terminal alkenyl group of the isobutylene polymer (A), the hydrosilyl group of the compound (C), and the carbon-carbon unsaturated bond functional group of the compound (D) will be described.

  In the sealing material composition of the present invention, as described above, the compound (C) having a hydrosilyl group is an isobutylene polymer (A) having an alkenyl group at the terminal and / or a carbon-carbon unsaturated bond functional group-containing compound. It is preferable that it is hydrolyzed with (D) and is in a bonded state. When the compound (C) is hydrosilylated with both components of the isobutylene polymer (A) and the compound (D), i) the compound (C) and the isobutylene polymer (A) are reacted, D) is added to react the compound (C) with the compound (D), ii) after reacting the compound (C) and the compound (D), the isobutylene polymer (A) is added, and the compound ( C) and a method of reacting the isobutylene polymer (A), iii) a method of reacting the isobutylene polymer (A) and the compound (D) with the compound (C) at the same time can be adopted. However, the method is not particularly questioned.

  Furthermore, in the sealing material composition of the present invention, it is preferable that the isobutylene polymer (A) is hydrosilylated and crosslinked by the compound (C). The hydrosilylation crosslinking with the compound (C) may be performed as long as a part of the isobutylene polymer (A) is crosslinked or may be completely crosslinked.

  Hydrosilylation crosslinking with the compound (C) of the isobutylene polymer (A) is achieved in a state where these two components are contained, but can also be achieved under conditions containing the compound (D). Further, the compound (D) and the compound (C) are reacted in advance by a hydrosilylation reaction to prepare the compound (C) functionalized with the compound (D), and then the hydrosilyl group remaining in the compound (C) A means for further bonding the terminal alkenyl group of the isobutylene polymer (A) by a hydrosilylation reaction may be employed, but the method is not particularly limited.

  The cross-linking of the isobutylene polymer (A) may be carried out at any stage, but from the viewpoint of the rigidity and rubber elasticity of the composition, it is dynamically cross-linked at the time of melt-kneading with the thermoplastic resin (B). It is preferable.

  In the present invention, the hydrosilylation reaction between the compound (C) and the isobutylene polymer (A) and / or the compound (D) proceeds by mixing and heating them. To proceed, a hydrosilylation catalyst as a reaction catalyst can be further added. Such a hydrosilylation catalyst is not particularly limited, and examples thereof include radical initiators such as organic peroxides and azo compounds, transition metal catalysts, and the like.

  The organic peroxide is not particularly limited. For example, di-t-butyl peroxide, 2,5-dimethyl-2,5-di (t-butylperoxy) hexane, 2,5-dimethyl-2,5-di Dialkyl peroxides such as (t-butylperoxy) -3-hexyne, dicumyl peroxide, t-butylcumyl peroxide, α, α′-bis (t-butylperoxy) isopropylbenzene, benzoyl peroxide, p-chlorobenzoyl peroxide , M-chlorobenzoyl peroxide, 2,4-dichlorobenzoyl peroxide, acyl peroxides such as lauroyl peroxide, peracid esters such as t-butyl perbenzoate, diisopropyl percarbonate, di-2-ethylhexyl percarbonate Peroxydicarbonate such as 1,1-di Examples thereof include peroxyketals such as (t-butylperoxy) cyclohexane and 1,1-di (t-butylperoxy) -3,3,5-trimethylcyclohexane.

  The azo compound is not particularly limited, and examples thereof include 2,2′-azobisisobutyronitrile, 2,2′-azobis-2-methylbutyronitrile, 1,1′-azobis-1-cyclohexanecarbonitrile, Examples include 2,2'-azobis (2,4-dimethylvaleronitrile), 2,2'-azoisobutyrovaleronitrile and the like.

Also, it is not particularly limited as a transition metal catalyst, for example, platinum simple substance, alumina, silica, carbon black or the like dispersed in a platinum solid, chloroplatinic acid, chloroplatinic acid and alcohol, aldehyde, ketone, etc. And platinum allylsiloxane such as platinum-olefin complex, platinum (0) -diallyltetramethyldisiloxane complex, and the like. Examples of the catalyst other than platinum _{compounds, RhCl (PPh 3) 3,} RhCl 3, RuCl 3, IrCl 3, FeCl 3, AlCl 3, PdCl 2 · H 2 O, NiCl 2, TiCl 4 , and the like. These catalysts may be used alone or in combination of two or more. Of these, platinum allylsiloxane is most preferred in terms of compatibility and reaction efficiency.

The amount of the hydrosilylation catalyst used is not particularly limited, but when the total number of moles of the alkenyl group of the isobutylene polymer (A) and / or the carbon-carbon unsaturated bond of the compound (D) is 1 mol, 10 may employed in the range of ^-1 to 10 ^-8 mol, and it is preferably employed in the range of 10 ^-2 to 10 ^-7 mol. When the amount is less than 10 ⁻⁸ mol, the hydrosilylation reaction tends not to proceed sufficiently. Moreover, since the hydrosilylation catalyst is expensive, it is preferable not to use more than 10 ⁻¹ mol.

The nitrogen atom-containing compound (E) has an effect of improving long-term adhesion with the substrate. Such nitrogen atom-containing compound (E) is not particularly limited as long as it has a functional group of amines, amides, hydrazines, and carboxylic acid hydrazides, but aminos include (—NH ₂ ) Group, (—NH—) group and the like; it may have an amino group; amides include (—CO · NH ₂ ) group, (—CO · NH—) group, ((—CO) _2. The hydrazines only need to have a hydrazide group such as a (—NH · NH ₂ ) group or (—NH · NH—) group; a carboxylic acid. The hydrazides may have a carboxylic acid hydrazide group such as a (—CO · NH · NH ₂ ) or (—CO · NH · NH—) group. These nitrogen-containing functional groups may be contained in at least one kind in one molecule, and may be contained in plural kinds. The functional group other than the amino group, amide group, hydrazide group, and carboxylic acid hydrazide group present in the nitrogen atom-containing compound (E) is not particularly limited as long as it can be used, but a vinyl group, a methacryl group, an acrylic group, Examples include mercapto group, hydroxyl group, isocyanate group, glycidyl group and the like.

Specific examples of such a nitrogen atom-containing compound (E) include: methylamine (CH ₃ · NH ₂ ), dimethylamine ((CH ₃ ) ₂ · NH), ethylenediamine (NH ₂ · CH ₂ · CH ₂ Acyclic amines such as NH ₂ ) and hexamethylene diamine (NH _2. (CH ₂ ) ₆ .NH ₂ ); saturated alicyclic amines; unsaturated alicyclic amines; cycloterpene amines; aniline (C ₆ H ₅ · NH ₂ ), chloroaniline (Cl · C ₆ H ₄ · NH ₂ ), diphenylamine ((C ₆ H ₅ ) ₂ · NH), 1-naphthylamine (C ₁₀ H ₇ · NH ₂ ), Aromatic amines such as phenylenediamine (C ₆ H ₄ (NH ₂ ) ₂ ) and benzidine (NH ₂ · C ₆ H ₄ · C ₆ H ₄ · NH ₂ ); monoaminoethanol (NH ₂ (C ₂ H ₄ Amino alcohols such as OH)); aminobenzaldehyde Amino aldehydes; aminoketones; glycine _{(NH 2 · CH 2 · COOH} ), sarcosine amino acids, such as _{(CH 3 · NH · CH 2} · COOH); hexanamide _{(C 5 H 11 · CO ·} NH 2), succinamide _{(H 2 N · CO · C} 2 H 4 · CO · NH 2), 4- acetamido benzoic acid _{(p- (CH 3 · CO ·} NH) · C 6 H 4 · COOH), adipic acid diamide (H ₂ Amides having N · CO · (CH ₂ ) ₄ · CO · NH ₂ ); Dicyandiamide (H ₂ N · C (NH) · NH · CN); 1,1-dimethyldiazine (H ₂ N · N) Hydrazines such as (CH ₃ ) ₂ ), 1,2-diphenyldiazine ((C ₆ H ₅ ) · NH · NH · (C ₆ H ₅ )); acetohydrazide (CH ₃ · CO · NH · NH ₂ ), benzohydrazide _{(C 6 H 5 · CO ·} NH · N _2), cyclohexane carbohydrazide _{(c-C 6 H 11 ·} CO · NH · NH 2), adipic acid dihydrazide _{(H 2 N · NH · CO} · (CH 2) 4 · CO · NH · NH 2), Isofuchiru acid dihydrazide _{(m-C 6 H 4 ·} (CO · NH · NH 2) 2) carboxylic acid hydrazides, such as and the like. Among these, hexamethylenediamine, benzidine, dicyandiamide, adipic acid dihydrazide, isophthalic acid dihydrazide and the like are preferable, and carboxylic acid dihydrazides such as dicyandiamide, adipic acid dihydrazide and isophthalic acid dihydrazide are particularly preferable in terms of glass adhesion.

  As for the nitrogen atom-containing compound (E), only one type may be used alone, or two or more types may be used in combination, and 100 parts by weight of the isobutylene polymer (A) having an alkenyl group at the terminal is used. , Preferably in the range of 0.01 to 50 parts by weight. In particular, it is preferably used in the range of 0.1 to 30 parts by weight.

  In addition, when the nitrogen atom-containing compound (E) is solid at room temperature, the particle diameter is preferably 1 mm or less, and more preferably 200 μm or less. When the particle size is 1 mm or more, the dispersibility is deteriorated, and good adhesiveness is hardly exhibited.

  The resin composition used for the rubber spacer constituting the double-glazed glass of the present invention is further blended with a tackifier resin (F) and an inorganic filler (G) as appropriate according to the required characteristics according to each application. be able to.

  The tackifier resin (F) is a low molecular resin having a number average molecular weight of 300 to 3,000 and a softening point of 60 to 150 ° C. based on the ring and ball method defined in JIS K-2207. Derivatives, polyterpene resins, aromatic modified terpene resins and their hydrides, terpene phenol resins, coumarone indene resins, aliphatic petroleum resins, alicyclic petroleum resins and their hydrides, aromatic petroleum resins and their hydrogen And a low molecular weight polymer of an aliphatic aromatic copolymer-based petroleum resin, a dicyclopentadiene-based petroleum resin and a hydride thereof, styrene or substituted styrene.

  Such a tackifier resin (F) has an effect of increasing hot melt adhesiveness. In order to achieve such an object, it is desirable to blend a tackifier resin (F) that is compatible with the isobutylene polymer (A). As such a tackifier resin (F), for example, an alicyclic petroleum resin and a hydride thereof, an aliphatic petroleum resin, a hydride of an aromatic petroleum resin, a polyterpene resin and the like are preferably used.

  Although the compounding quantity of tackifying resin (F) is not specifically limited, It is preferable that it is 1-300 weight part with respect to 100 weight part of isobutylene polymer (A), From the point of coexistence of gas barrier property and adhesiveness, More preferably, it is 1-100 weight part.

  The inorganic filler (G) has an effect of improving the rigidity of the rubber spacer in the present invention, has an effect of improving shape maintainability in the use temperature range, and suppresses dripping during hot melt. There is no restriction | limiting in particular as an inorganic filler (G), A conventionally well-known thing can be used. For example, calcium carbonate, magnesium carbonate, fused silica, crystalline silica, diatomaceous earth, clay, talc, mica, kaolin, titanium oxide, zinc oxide, carbon black, bentonite, aluminum hydroxide, magnesium hydroxide, barium sulfate, calcium sulfate, etc. At least one selected from the group consisting of can be used. Among these, carbon black having an effect of improving rigidity in a small amount is particularly preferable.

  The blending amount of the inorganic filler (G) is preferably 1 to 200 parts by weight with respect to 100 parts by weight of the isobutylene polymer (A). This is because when a large amount of the inorganic filler (G) is added, the fluidity at the time of hot melt deteriorates.

  An alkoxysilane compound can be further added to the resin composition used for the rubber spacer 4 of the present invention. An alkoxysilane compound is a compound having an alkoxysilyl group, has an effect of improving long-term adhesion with a substrate, and can be used as appropriate according to required characteristics. The alkoxysilyl group species is not particularly limited as long as it can be used, and examples thereof include those having a hydrolyzable group such as a methoxysilyl group, an ethoxysilyl group, a propoxysilyl group, and an oximesilyl group. The functional group other than the alkoxysilyl group present in the alkoxysilane compound is not particularly limited as long as it can be used, but vinyl group, methacryl group, acrylic group, mercapto group, hydroxyl group, isocyanate group, amino group, amide group, Examples include glycidyl groups. More specific examples include ethyl silicate, silicate condensate, vinyltrimethoxysilane, 3-methacryloxypropyltrimethoxysilane, 3-aminopropyltrimethoxysilane, 3-aminopropylmethyldimethoxysilane, 3-aminopropylmethyldi Ethoxysilane, 3-aminopropyltriethoxysilane, N-methyl-3-aminopropyltrimethoxysilane, N-phenyl-3-aminopropyltrimethoxysilane, N- (β-aminoethyl) aminopropylmethyldimethoxysilane, 3 -Isocyanatopropyltrimethoxysilane, 3-isocyanatopropyltriethoxysilane, 3-glycidylpropyltrimethoxysilane and the like are exemplified. Among these, an alkoxysilane compound having an amino group, an isocyanate group, or an epoxy group is particularly preferable in terms of improving the glass adhesion of the rubber spacer 4.

  As the alkoxysilane compound, only one kind may be used alone, or two or more kinds may be used in combination. The range is 0.01 to 50 parts by weight with respect to 100 parts by weight of the isobutylene polymer (A). Is preferably used. In particular, it is preferably used in the range of 0.1 to 30 parts by weight.

  A plasticizer can be further added to the resin composition used for the rubber spacer 4 of the present invention. Plasticizers include paraffinic process oil, naphthenic process oil, petroleum process oil such as aromatic process oil, dibasic acid dialkyl such as diethyl phthalate, dioctyl phthalate and dibutyl adipate, liquid polybutene, liquid poly Low molecular weight liquid polymers such as isobutylene and liquid polyisoprene are exemplified, and any of these can be used. Such a plasticizer has an effect of improving fluidity at the time of hot melt, and in order to achieve such an object and prevent bleed out, a plasticizer compatible with the isobutylene polymer (A). Is desirable, and paraffinic process oil, liquid polybutene, liquid polyisobutylene, and the like are preferably used.

  Although the compounding quantity of a plasticizer is not specifically limited, Usually, it is 1-300 weight part with respect to 100 weight part of isobutylene polymer (A), Preferably it is 1-100 weight part.

  A desiccant can be further added to the resin composition used for the rubber spacer 4 of the present invention. Examples of the desiccant include zeolite, silica gel, and alumina, and any of these can be used. Such a desiccant can reduce the water vapor permeability of the rubber spacer 4 and prevent the hollow layer 5 sandwiched between the glass plates 2 and 3 of the multilayer glass from being clouded by moisture. The blending amount of the desiccant is preferably 1 to 100 parts by weight with respect to 100 parts by weight of the isobutylene polymer (A).

  In addition, the resin composition used for the rubber spacer 4 of the present invention is appropriately blended with an antioxidant, an ultraviolet absorber, a light stabilizer, a pigment, a surfactant, a flame retardant and the like as long as the physical properties are not impaired. be able to. Known antiblocking agents, antistatic agents, colorants, inorganic or organic antibacterial agents, lubricants, and the like can also be added.

  Examples of the antioxidant include generally used antioxidants such as phenol, amine, sulfur, phosphorus, hydrazine, and amide. Phenols and amines prohibit radical chaining and are used as primary antioxidants. Examples of phenolic antioxidants include 2,6-di-t-butyl-p-cresol and 2,6-diphenyl- 4-octoxyphenol, stearyl- (3,5-dimethyl-4-hydroxybenzyl) thioglycolate, stearyl-β- (4-hydroxy-3,5-di-t-butylphenyl) propionate, distearyl-3, 5-di-t-butyl-4-hydroxybenzylphosphonate, 2,4,6-tris (3 ', 5'-di-t-butyl-4-hydroxybenzylthio) 1,3,5-triazine, distearyl (4-Hydroxy-3-methyl-5-t-butyl) benzyl malonate, 2,2'-methylenebis (4-methyl-6-t-butylphenol) 4,4'-methylenebis (2,6-di-t-butylphenol), 2,2'-methylenebis [6- (1-methylcyclohexyl) p-cresol], bis [3,5-bis ( 4-hydroxy-3-t-butylphenyl) butyric acid] glycol ester, 4,4'-butylidenebis (6-t-butyl-m-cresol), 2,2'-ethylidenebis (4,6-di-) t-butylphenol), 2,2'-ethylidenebis (4-s-butyl-6-t-butylphenol), 1,1,3-tris (2-methyl-4-hydroxy-5-t-butylphenyl) Butane, bis [2-tert-butyl-4-methyl-6- (2-hydroxy-3-tert-butyl-5-methylbenzyl) phenyl] terephthalate, 1,3,5-tris (2,6-dimethyl) Ru-3-hydroxy-4-t-butyl) benzyl isocyanurate, 1,3,5- (3,5-di-t-butyl-4-hydroxybenzyl) -2,4,6-trimethylbenzene, tetrakis [ Methylene-3- (3,5-di-tert-butyl-4-hydroxyphenyl) propionate] methane, 1,3,5-tris (3,5-di-tert-butyl-4-hydroxybenzyl) isocyanurate, 1,3,5-tris [(3,5-di-t-butyl-4-hydroxyphenyl) propionyloxyethyl] isocyanurate, 2-octylthio-4,6-di (4-hydroxy-3,5-di -T-butyl) phenoxy-1,3,5-triazine, 4,4'-thiobis (6-t-butyl-m-cresol), 2,2'-methylenebis (6-t-butyl-4-methyl) Phenol) monoacrylate, triethylene glycol bis [3- (3-t-butyl-4-hydroxy-5-methylphenyl) propionate], 3,9-bis (1,1-dimethyl-2-hydroxyethyl) 2, 4,8,10-tetraoxaspiro [5,5] undecanbis [3- (3-t-butyl-4-hydroxy-5-methylphenyl) propionate] and the like. These may be used alone or in combination of two or more.

  Examples of amine-based antioxidants include phenyl-α-naphthylamine, phenyl-β-naphthylamine, N, N′-diphenyl-p-phenylenediamine, N, N′-di-β-naphthyl-p-phenylenediamine, N-cyclohexyl-N′-phenyl-p-phenylenediamine, N-phenylene-N′-isopropyl-p-phenylenediamine, 6-ethoxy-2,2,4-trimethyl-1,2-dihydroquinoline, 2, Examples thereof include polymers composed of 2,4-trimethyl-1,2-dihydroquinoline. These may be used alone or in combination of two or more.

  Sulfur-based and phosphorus-based antioxidants are used as secondary antioxidants by decomposing peroxides. Examples of sulfur-based antioxidants include thiobis (β-naphthol), thiobis (N-phenyl-). β-naphthylamine), 2-mercaptobenzothiazole, 2-mercaptobenzimidazole, dodecyl mercaptan, dilauryl thiodipropionate, distearyl thiodipropionate, pentaerythritol tetralauryl thiopropionate, tetramethylthiuram monosulfide, tetra Examples thereof include methyl thiuram disulfide, nickel dibutyl dithiocarbamate, nickel isopropyl xanthate, dioctadecyl sulfide, and the like. These may be used alone or in combination of two or more.

  Examples of phosphorus antioxidants include trioctyl phosphite, trilauryl phosphite, tridecyl phosphite, octyl-diphenyl phosphite, tris (2,4-di-t-butylphenyl) phosphite, triphenyl phosphite. Phyto, tris (butoxyethyl) phosphite, tris (nonylphenyl) phosphite, distearyl pentaerythritol diphosphite, tetra (tridecyl) -1,1,3-tris (2-methyl-5-t-butyl-4 -Hydroxyphenyl) butanediphosphite, tetra (C12-15 mixed alkyl) -4,4'-isopropylidenediphenyldiphosphite, tetra (tridecyl) -4,4'-butylidenebis (3-methyl-6-t- Butylphenol) diphosphite, tris (3 -Di-t-butyl-4-hydroxyphenyl) phosphite, tris (mono-dimixed nonylphenyl) phosphite, hydrogenated-4,4'-isopropylidenediphenol polyphosphite, bis (octylphenyl) bis [4,4′-butylidenebis (3-methyl-6-tert-butylphenol), 1,6-hexanediol diphosphite phenyl, 4,4′-isopropylidenediphenol, pentaerythritol diphosphite, bis (2, 4-di-t-butylphenol) pentaerythritol diphosphite, bis (2,6-di-t-butyl-4-methylphenyl) pentaerythritol diphosphite, tris [4,4'-isopropylidenebis (2- t-butylphenol)] phosphite, phenyl diisodecylphosphine Ito, di (nonylphenyl) pentaerythritol diphosphite, tris (1,3-distearoyloxyisopropyl) phosphite, 4,4'-isopropiodenbis (2-tert-butylphenol) dinonylphenyl phosphite, 9 , 10-dihydro-9-oxa-10-phosphaphenanthrene-10-oxide, tetrakis (2,4-di-t-butylphenyl) -4,4'-biphenylene diphosphite, and the like. These may be used alone or in combination of two or more.

  Hydrazine-based and amide-based antioxidants have the property of preventing radical initiation, and examples thereof include N-salicyloyl-N′-aldehyde hydrazine, N, N′-diphenyl oxide, and the like.

  These antioxidants may be used alone or in combination of two or more regardless of the type. Furthermore, citric acid, phosphoric acid, etc. are mentioned as what improves an antioxidant effect by using together with antioxidant.

  As the ultraviolet absorber, commonly used ultraviolet absorbers such as 2-hydroxybenzophenone, 2,4-dihydroxybenzophenone, 2,2 ', 4-trihydroxybenzophenone, 2,2', 4,4'- Tetrahydroxybenzophenone, 2-hydroxy-4-methoxybenzophenone, 2-hydroxy-4-octoxybenzophenone, 2-hydroxy-4-methylbenzophenone, 2-hydroxy-4-chlorobenzophenone, 2,2'-dihydroxy-4- Benzophenone series such as methoxybenzophenone and 2,2'-dihydroxy-44'-dimethoxybenzophenone; phenylsulcylate, 2,4-di-t-butylphenyl-3,5-di-t-butyl-4-hydroxybenzoate Saltylate type such as 2- (5- 2-hydroxyphenyl) benzotriazole, 2- [2-hydroxy-3,5-bis (α, α-dimethylbenzyl) phenyl] 2H-benzotriazole, 2- (3,5-di-t-butyl- 2-hydroxyphenyl) benzotriazole, 2- (3-tert-butyl-5-methyl-2-hydroxyphenyl) -5-chlorobenzotriazole, 2- (3,5-di-tert-butyl-2-hydroxyphenyl) ) -5-chlorobenzotriazole, 2- (3,5-di-t-amyl-2-hydroxyphenyl) -5-chlorobenzotriazole, 2- (2'-hydroxy-5'-t-octylphenyl) benzo Benzotriazoles such as triazole; ethyl-2-cyano-3,3-diphenyl acrylate, methyl-2-carbomethoxy-3- (p Acrylonitrile such as methoxyphenyl) acrylate. Benzotriazole are preferred among these. These ultraviolet absorbers may be used alone or in combination of two or more.

  As the light stabilizer, commonly used light stabilizers such as bis (2,2,6,6-tetramethyl-4-piperidyl) sebacate, bis (1,2,2,6,6-pentamethyl- 4-piperidyl) sebacate, 1,2,3,4-tetrakis (2,2,6,6-tetramethyl-4-piperidyloxycarbonyl) butane, 1,2,3,4-tetrakis (1,2,2 , 6,6-pentamethyl-4-piperidyloxycarbonyl) butane, dimethyl-1- (2-hydroxyethyl) -4-hydroxy-2,2,6,6-tetramethylpiperidine polycondensate, 2- ( 3,5-di-tert-butyl-4-hydroxybenzyl) -2-n-butylmalonate bis (1,2,2,6,6-pentamethyl-4-piperidyl), 1,2,3,4-butane -Tetraca Boronic acid, 1,2,2,6,6 pentamethyl-4-piperidinol and 3,9-bis (2-hydroxy-1,1-dimethylethyl) -2,4,8,10-tetraoxospiro [ 5,5] polycondensate of undecane, 1- (3,5-di-tert-butyl-4-hydroxyphenyl) -1,1-bis (2,2,6,6-tetramethyl-4-piperidyloxy) Carbonyl) pentane, 1- [2- [3- (3,5-di-t-butyl-4-hydroxyphenyl) propionyloxy] ethyl] -4- [3- (3,5-di-t-butyl- 4-hydroxyphenyl) propionyloxy] -2,2,6,6-tetramethylpiperidine, N, N′-bis (3-aminopropyl) ethylenediamine · 2,4-bis [N-butyl-N- (1, 2,2,6,6-pentamethyl- Piperidyl) amino] -6-chloro-1,3,5-triazine condensate, 4-benzoyloxy-2,2,6,6-tetramethylpiperidine, poly [{6- (1,1,3,3- Tetramethylbutyl) amino-1,3,5-triazine-2,4-diyl} {(2,2,6,6-tetramethyl-4-piperidyl) imino} hexamethylene {(2,2,6,6 -Tetramethyl-4-piperidyl) imino}], bis (1-octyloxy-2,2,6,6-tetramethyl-4-piperidyl) sebacate and the like. These may be used alone or in combination of two or more.

  The method for producing the resin composition used for the rubber spacer in the present invention is not particularly limited, and mechanically using a roll, a Banbury mixer, a kneader, a melting pot equipped with a stirrer, or a single or twin screw extruder. Can be used. At this time, it is also possible to heat as necessary. Moreover, after adding a compounding agent to a suitable solvent and stirring this, after obtaining the uniform solution of a composition, the method of distilling a solvent off can also be used.

  Resin composition used for rubber spacer of the present invention by dynamically crosslinking isobutylene polymer (A) with compound (C) during melt mixing of isobutylene polymer (A) and thermoplastic resin (B) When manufacturing a thing, it can carry out preferably by the method illustrated below. For example, when producing using a closed kneading apparatus or a batch kneading apparatus such as a lab plast mill, Brabender, Banbury mixer, kneader, roll, etc., all components other than the compounds (C) and (E) are added. It is possible to employ a method in which the mixture is melt-kneaded until uniform, the compound (C) is added and the crosslinking reaction proceeds sufficiently, and then the compound (E) is added and further kneaded to stop the melt-kneading.

  Moreover, when manufacturing using a continuous melt-kneading apparatus like a single-screw extruder, a twin-screw extruder, etc., (1) All components other than a compound (C) and (E) are made into an extruder beforehand. After melt-kneading until uniform by a melt-kneading apparatus such as pellets, dry blending compound (C), and then melt-kneading with a melt-kneading apparatus such as an extruder, isobutylene polymer (A) By dynamically crosslinking and adding the compound (E) from the middle of the cylinder of the extruder and further melt-kneading, or (2) the compound (C) having at least two hydrosilyl groups in the molecule And all components other than (E) are melt-kneaded by a melt-kneading apparatus such as an extruder, and a compound (C) having at least two hydrosilyl groups in the molecule is added to the middle of the cylinder of the extruder. Then, the isobutylene polymer (A) having an alkenyl group at the terminal is dynamically cross-linked, and the compound (E) is added to the middle of the cylinder of the extruder and further melt-kneaded. A method for producing the composition can be employed.

  The kneading conditions for carrying out the above-described method of performing dynamic crosslinking simultaneously with melt-kneading may be at or above the temperature at which the thermoplastic resin (B) melts, and preferably 260 ° C. or below.

  The rubber spacer 4 of the present invention comprising the resin composition as described above is excellent in gas barrier properties, has hot-melt adhesiveness and long-term adhesion durability, and also has a sealing function. No sealing material is required.

  Next, the resin used for the resin spacer 6 is not particularly limited, and various synthetic resin materials can be used. Both hard resin materials and soft resin materials can be used. From the viewpoint of long-term durability, a hard resin material is preferable. Moreover, although both a thermoplastic resin and a thermosetting resin can be used, a thermoplastic resin is preferable from the viewpoint of simplifying the manufacturing process of the double-glazed glass. Moreover, the foam of these resin materials can also be used. Examples of resins that can be used include olefin resins such as polyethylene and polypropylene, styrene resins such as polystyrene, halogenated olefin resins, polyester resins, acrylic resins, polyamide resins, silicone resins, polycarbonate resins, and urethanes. Various resin materials such as epoxy resin and epoxy resin are listed. Furthermore, those modified bodies, copolymers, mixtures, polymer alloys and the like can also be used. Among these various synthetic resin materials, olefin-based resins such as polyethylene and polypropylene are preferable from the viewpoint of simplifying the production process of the double-glazed glass. Also, butyl rubber mainly composed of isobutylene and isobutylene, brominated butyl rubber and the like. Butyl rubber can also be used.

In particular, the resin spacer 6 contains a desiccant and, when provided on the inner peripheral side of the rubber spacer 4, the water vapor permeability is 1 g · cm / m ² under the conditions of 40 ° C. and relative humidity 90%. -It is preferable to have a moisture permeability greater than 24 hr, and when the moisture permeability of the resin material itself is small, it is possible to achieve this numerical value with the structure of the molded body such as foaming or open celling.

  As the desiccant contained in the resin spacer 6, those usually used for multilayer glass such as zeolite, alumina and silica gel are used. Typical zeolites include natural zeolites and synthetic zeolites such as Union Carbite molecular sieves 3A, 4A, 5A, 13X, and 15X. The desiccant is preferably kneaded and dispersed in the resin during molding of the resin spacer 6.

  The content of the desiccant in the resin spacer 6 is preferably 20% by weight or more. If the content of the desiccant is less than 20% by weight, the purpose of adding the desiccant that prevents the hollow layer 5 sandwiched between the glass plates 2 and 3 of the multilayer glass 1 from being clouded by moisture may not be sufficiently achieved. is there. Moreover, when there is too much content of desiccants, such as a zeolite, it exists in the tendency for the melt viscosity of the resin spacers 6 to rise, and for moldability to fall. Therefore, it is preferable that the addition amount of a desiccant is 20 to 50 weight%, More preferably, it is the range of 20 to 40 weight%.

  Moreover, it does not specifically limit as hot-melt resin used for the sealing material 7 which consists of hot-melt resin which has moisture permeability, Although various hot-melt resin can be used, moisture permeability and hot-melt adhesiveness are not limited. From the viewpoint, for example, EVA, EEA, EAA and the like are preferable. Further, the sealing material 7 preferably has hot melt properties so as to be molded and applied at the same time as the rubber spacer 4. A sealant can also be used.

The sealing material 7 contains a desiccant and is provided on the inner peripheral side of the rubber spacer 4 and has a water vapor transmission rate of 1 g · cm / m ² · 24 hr under conditions of 40 ° C. and a relative humidity of 90%. It is preferred to have greater moisture permeability.

  As the desiccant contained in the sealing material 7, the same zeolite, alumina, silica gel and the like as described above are used. The desiccant is preferably kneaded and dispersed in the resin when the sealing material 7 is molded.

  The content of the desiccant in the sealing material 7 is preferably 20% by weight or more. If the content of the desiccant is less than 20% by weight, the purpose of adding the desiccant that prevents the hollow layer 5 sandwiched between the glass plates 2 and 3 of the multilayer glass 1 from being clouded by moisture may not be sufficiently achieved. is there. Moreover, when there is too much content of desiccants, such as a zeolite, the hot-melt adhesiveness of the sealing material 7 falls. Therefore, it is preferable that the addition amount of a desiccant is 20 to 50 weight%, More preferably, it is the range of 20 to 40 weight%.

  Hereinafter, the present invention will be described in more detail based on examples, but the present invention is not limited by these.

(Production Example 1) [Production of isobutylene polymer (APIB) having an alkenyl group at the terminal]
A 2 L separable flask was fitted with a three-way cock, thermocouple, and stirring seal, and purged with nitrogen. After nitrogen substitution, nitrogen was flowed using a three-way cock. To this, 785 ml of toluene and 265 ml of ethylcyclohexane were added using a syringe. After adding the solvent, the water content was measured with a Karl Fischer moisture meter. After the measurement, the mixture was cooled to about −70 ° C., and 277 ml (2933 mmol) of isobutylene monomer was added thereto. After cooling to about −70 ° C. again, 0.85 g (3.7 mmol) of p-dicumyl chloride and 0.68 g (7.4 mmol) of picoline were dissolved in 10 ml of toluene and added. When the internal temperature of the reaction system became -74 ° C and stabilized, 19.3 ml (175.6 mmol) of titanium tetrachloride was added to initiate polymerization. When the polymerization reaction was completed (90 minutes), 1.68 g (11.0 mmol) of a 75% allyltrimethylsilane / toluene solution was added, and the reaction was further continued for 2 hours. Then, it is deactivated with pure water heated to about 50 ° C., the organic layer is further washed with pure water (70 ° C. to 80 ° C.) three times, the organic solvent is removed at 80 ° C. under reduced pressure, and the number average molecular weight is increased. An isobutylene polymer containing 2.0500 terminal allyl groups per molecule was obtained.
The number average molecular weight in the present specification was measured by a Waters 510 type GPC system (chloroform was used as a solvent and the flow rate was 1 mL / min), and the value in terms of polystyrene was shown.

(Production Example 2) [Production of styrene-isobutylene-styrene triblock copolymer (SIBS)]
After replacing the inside of the polymerization vessel of the 2 L separable flask with nitrogen, 456.1 mL of n-hexane (dried with molecular sieves) and 656.5 mL of butyl chloride (dried with molecular sieves) were added using a syringe. After the polymerization vessel was cooled in a dry ice / methanol bath at −70 ° C., a Teflon (registered trademark) feeding tube was attached to a pressure-resistant glass liquefied collection tube with a three-way cock containing 232 mL (2871 mmol) of isobutylene monomer. Then, isobutylene monomer was fed into the polymerization vessel by nitrogen pressure. 0.647 g (2.8 mmol) of p-dicumyl chloride and 1.22 g (14 mmol) of N, N-dimethylacetamide were added. Next, 8.67 mL (79.1 mmol) of titanium tetrachloride was further added to initiate polymerization. After stirring at the same temperature for 1.5 hours from the start of polymerization, about 1 mL of the polymerization solution was extracted from the polymerization solution for sampling. Subsequently, a mixed solution of 77.9 g (748 mmol) of styrene monomer, 23.9 mL of n-hexane and 34.3 mL of butyl chloride, which had been cooled to −70 ° C. in advance, was added to the polymerization vessel. 45 minutes after the addition of the mixed solution, about 40 mL of methanol was added to terminate the reaction.
After distilling off the solvent from the reaction solution, it was dissolved in toluene and washed twice with water. Further, a toluene solution was added to a large amount of methanol to precipitate a polymer, and the obtained polymer was vacuum-dried at 60 ° C. for 24 hours to obtain a target isobutylene triblock copolymer. The number average molecular weight of the isobutylene polymer before addition of styrene was 50,000, and the number average molecular weight of the block copolymer after styrene polymerization was 67,000.

(Production Example 3) [Production of styrene-isobutylene-diblock copolymer (SIB)]
After replacing the inside of the polymerization container of the 500 mL separable flask with nitrogen, add 84.9 mL of n-hexane (dried with molecular sieves) and 122.2 mL of butyl chloride (dried with molecular sieves) using a syringe. After the polymerization vessel was placed in a dry ice / methanol bath at -70 ° C and cooled, a Teflon (registered trademark) made of pressure-resistant glass-made liquefied collection tube with a three-way cock containing 78.3 mL (828.8 mmol) of isobutylene monomer was added. A liquid feeding tube was connected, and isobutylene monomer was fed into the polymerization vessel by nitrogen pressure. 0.217 g (1.4 mmol) of cumyl chloride and 0.12 g (1.4 mmol) of N, N-dimethylacetamide were added. Next, 1.54 mL (14.0 mmol) of titanium tetrachloride was further added to initiate polymerization. After stirring for 120 minutes from the start of polymerization, about 1 mL of the polymerization solution was extracted from the polymerization solution for sampling. Subsequently, 9.48 g (91.0 mmol) of styrene monomer was added into the polymerization vessel. 45 minutes after adding the mixed solution, the reaction was terminated by adding a large amount of water.
The reaction solution was washed twice with water, the solvent was evaporated, and the resulting polymer was vacuum-dried at 60 ° C. for 24 hours to obtain the desired isobutylene diblock copolymer. The number average molecular weight was 48,000.

(Examples 1 to 10 and Comparative Examples 1 and 2)
Rubber spacer: The isobutylene polymer (A), the thermoplastic resin (B), the hydrosilylation catalyst, and the compound (D) were melt-mixed in advance at a ratio shown in Table 1 at 120 ° C. or less. Compound (C) was added to this mixture in the ratio shown in Table 1, and sufficiently melt-kneaded using a lab plast mill (manufactured by Toyo Seiki Co., Ltd.). Thereafter, by further melt-kneading the nitrogen atom-containing compound (E), tackifier resin (F), inorganic filler (G), and desiccant in the proportions shown in Table 1 at 100 to 180 ° C., A resin composition to be a rubber spacer was manufactured.
Resin spacer: A resin composition was prepared by melting and kneading for 15 minutes using a lab plast mill (manufactured by Toyo Seiki Seisakusho Co., Ltd.) at a ratio shown in Table 1 at 170 ° C.

[Manufacture of moisture permeability test pieces]
The obtained resin composition of Example 2 was heated and pressed at 140 ° C. to produce a 1 mm thick sheet.

[Manufacture of test specimens for shape maintenance, glass tackiness, and adhesion retention]
Each obtained resin composition was heat-pressed under the conditions of 100 to 170 ° C. and molded into a width of 10 mm × 50 mm. At this time, each was molded with the thickness shown in Table 1. This test piece was sandwiched between two glass plates of 50 mm width × 50 mm length × 5 mm thickness, and cured for 10 minutes in an oven at 100 to 170 ° C. to produce a test piece. For Examples 3 to 6 and Comparative Example 2, the molded spacers were superposed at room temperature and sandwiched between glass plates in the same manner as described above to produce test pieces. Regarding Example 7, when the rubber spacer resin composition was molded to a thickness of 10 mm, a 5 mm thick aluminum spacer was inserted in advance, and the molding as shown in FIG. 11 had a width of 10 mm × 50 mm × 10 mm. Got the body. This was sandwiched between glass plates in the same manner as described above to produce test pieces.

[Evaluation methods]
(Moisture permeability)
In accordance with JIS Z 0208, moisture permeability was measured for the composition of Example 2 at 40 ° C. and 90% RH. As a result, it was 0.4 g / m ² · 24 h.
(Shape maintenance test)
A glass plate on one side is fixed, a load of 3 kg is applied to the other glass plate for 15 minutes, the amount of downward movement of the glass plate on the loaded side is measured under a temperature condition of 25 ° C., and the amount of movement is 0.5 mm or less. The thing was set as (circle) and the thing beyond it was set as x. The results are shown in Table 1.
(Glass tack test)
With the distance between the two glass plates stretched and deformed by 10% at the initial stage (after production), the glass plate was left for 15 minutes at a temperature of 25 ° C., and the degree of adhesion between the glass and the material interface was observed, and the bonding area was deformed. Those that did not change from before (initial) were marked with ◯, and those with peeling were marked with ×. The results are shown in Table 1.
(Adhesion retention test)
After immersing the test piece in warm water at 80 ° C. for 1 week, the glass adhesion test is performed, the degree of adhesion between the glass and the material interface is observed, and the same as before the bonding area is deformed (initial) The case where peeling was observed was taken as x. The results are shown in Table 1.

  In addition, the symbol of the material used by the Example and the comparative example below, and the specific content are as follows.

APIB: Isobutylene polymer having an alkenyl group at the terminal (Production Example 1)
SIBS: Styrene-isobutylene-styrene triblock copolymer (Production Example 2)
SIB: Styrene-isobutylene-diblock copolymer (Production Example 3)
PE: Polyethylene (Hi-Zex (registered trademark) 2200J, manufactured by Mitsui Chemicals, Inc.)
TPU: Thermoplastic polyurethane elastomer (Pandex (registered trademark) T-1375, manufactured by Dick Bayer Polymer Co., Ltd.)
IIR: Butyl rubber (Butyl 065, manufactured by JSR Corporation)
Si-H group (hydrosilyl group) containing compound: Polysiloxane (CH _{3) 3} SiO- represented by the chemical formula _{[Si (H) (CH 3} ) O] 40 -Si (CH 3) 3
ADH: Adipic acid dihydrazide (manufactured by Nippon Hydrazine Industry Co., Ltd.)
Petroleum resin: (Arcon (registered trademark) P-100, manufactured by Arakawa Chemical Industries, Ltd.)
Polyisobutylene: (Idemitsu Polybutene 300H, manufactured by Idemitsu Kosan Co., Ltd.)
CB: Carbon black (F200, manufactured by Asahi Carbon Co., Ltd.)
Calcium carbonate: (Softon 3200, manufactured by Bihoku Powder Chemical Co., Ltd.)
Zeolite: (PURMOL 3ST, manufactured by ZEOCHEM)
Catalyst Pt: 1,1,3,3-tetramethyl-1,3-dialkenyldisiloxane complex of zerovalent platinum, 3% by weight xylene solution PP: Polypropylene (Grand Polypro J215W, manufactured by Grand Polymer)
SEPS: Styrene-ethylenepropylene-styrene triblock copolymer (SEPTON 2007, manufactured by Kuraray Co., Ltd.)

  Among the spacer materials made of the resin composition containing the isobutylene polymer (A) constituting the multilayer glass of the present invention, the resin composition of Example 4 showed a good value of 0.4 for moisture permeability. . Moreover, as shown by the results of Examples 1 to 10, the spacer material constituting the multilayer glass of the present invention was excellent in shape maintenance, tackiness, and adhesion retention. On the other hand, Comparative Example 1, which is a spacer using a composition not containing the components (C) to (E), has good initial tackiness, but is inferior in shape maintainability. It turns out that it cannot be used. In Comparative Example 2 in which a rubber spacer mainly composed of butyl rubber and a resin spacer were used in combination, the initial adhesiveness and shape maintainability were good, but they were easily peeled after the hot water resistance test, and the adhesion retention was poor.

It is sectional drawing of the multilayer glass of 1st Embodiment. It is a fragmentary sectional view of the peripheral part of the multilayer glass of 1st Embodiment. It is a fragmentary sectional view of the peripheral part of the multilayer glass of 2nd Embodiment. It is a fragmentary sectional view of the peripheral part of the multilayer glass of 3rd Embodiment. It is a fragmentary sectional view of the peripheral part of the multilayer glass of 4th Embodiment. It is a fragmentary sectional view of the peripheral part of the multilayer glass of 5th Embodiment. It is a fragmentary sectional view of the peripheral part of the multilayer glass of 6th Embodiment. It is a fragmentary sectional view of the peripheral part of the multilayer glass of 7th Embodiment. It is a fragmentary sectional view of the peripheral part of the multilayer glass of 8th Embodiment. It is a fragmentary sectional view of the peripheral part of the multilayer glass of 9th Embodiment. It is a fragmentary sectional view of the peripheral part of the multilayer glass of 10th Embodiment. It is a fragmentary sectional view of the peripheral part of the multilayer glass of 11th Embodiment. It is a fragmentary sectional view of the peripheral part of the multilayer glass of 12th Embodiment. It is a fragmentary sectional view of the peripheral part of the multilayer glass of 13th Embodiment. It is a top view of the glass plate which shows arrangement | positioning of a spacer. It is a top view of the glass plate which shows arrangement | positioning of a spacer. An embodiment of the joint part of a spacer is shown, (a) is a perspective view and (b) is a top view. The other embodiment of the joint part of a spacer is shown, (a) is a perspective view, (b) is a top view. The other embodiment of the joint part of a spacer is shown, (a) is a top view of the spacer which abbreviate | omitted one part, (b) is a top view in the state which provided the said spacer in the glass plate, (c) is extrusion molding Explanatory drawing which shows the manufacturing method of the spacer by (a), (d) And (e) is a top view of the joint part of the spacer of other embodiment. The conventional multilayer glass is shown, (a) is sectional drawing, (b) is a fragmentary sectional view of a peripheral part.

Explanation of symbols

DESCRIPTION OF SYMBOLS 1 Multi-layer glass 2, 3 Glass plate 4 Rubber spacer 5 Hollow layer 6 Resin spacer 7 Seal material 8 Metal spacer 10 Seam 11 Connection piece 12 Sealing member 13 Die 14 Spacer 15 Primary seal material 16 Space | gap (recessed part)
17 Secondary sealant

Claims (14)

  In the multi-layer glass in which a plurality of glass plates are arranged to face each other at a predetermined interval via a spacer provided on the peripheral edge of the glass plate so as to form a hollow layer between them, the spacer has a terminal end. A rubber spacer having hot-melt adhesiveness containing an isobutylene polymer (A) having an alkenyl group, a thermoplastic resin (B), and a compound (C) having at least two hydrosilyl groups in the molecule. Multi-layer glass characterized by   The multilayer glass according to claim 1, wherein the rubber spacer further contains a compound (D) having a carbon-carbon unsaturated bond functional group, which is different from the component (A). .   The carbon-carbon unsaturated bond functional group-containing compound (D) further comprises an epoxy group, an alkoxy group, a radical polymerizable unsaturated group, a carboxyl group, a carboxylic acid anhydride group, a halogen atom, and an alkoxysilyl group. It has at least 1 sort (s) of functional group chosen from a group, The multilayer glass of Claim 2 characterized by the above-mentioned.   The multilayer glass according to any one of claims 1 to 3, wherein the rubber spacer further contains a nitrogen atom-containing compound (E).   The isobutylene polymer (A) having an alkenyl group at the terminal contained in the rubber spacer is crosslinked with a compound (C) having at least two hydrosilyl groups in the molecule. The multilayer glass in any one of 1-4.   The thermoplastic resin (B) contained in the rubber spacer is thermoplastic elastomer, polyethylene, polypropylene, ethylene-α olefin copolymer, polyisobutylene, isobutylene-isoprene copolymer (butyl rubber), chlorinated butyl, bromine. 2. It is at least one selected from the group consisting of brominated butyl, isobutylene- (p-methylstyrene) copolymer, and bromide of isobutylene- (p-methylstyrene) copolymer. The multilayer glass according to any one of 5.   The multilayer glass according to claim 6, wherein the thermoplastic elastomer is a styrene thermoplastic elastomer and / or a urethane thermoplastic elastomer.   An isobutylene block copolymer comprising the polymer block (a) having an aromatic vinyl compound as a constituent monomer and the polymer block (b) having an isobutylene as a constituent monomer. The multi-layer glass according to claim 7, which is a coalesced (B1).   The multilayer glass according to any one of claims 1 to 8, wherein a resin spacer is further provided on an inner peripheral side and / or an outer peripheral side of the rubber spacer.   The multilayer glass according to claim 9, wherein the resin spacer is made of a resin composition containing 20% by weight or more of a desiccant.   The multilayer glass according to any one of claims 1 to 10, wherein a sealing material made of a moisture-permeable hot melt resin containing a desiccant is provided on the inner peripheral side of the rubber spacer.   The multilayer glass according to any one of claims 1 to 11, wherein a metal spacer is further provided on an inner peripheral side and / or an outer peripheral side of the rubber spacer.   A resin composition having hot-melt adhesiveness containing an isobutylene-based polymer (A) having an alkenyl group at the end, a thermoplastic resin (B), and a compound (C) having at least two hydrosilyl groups in the molecule, Extrusion-molded into a predetermined spacer shape on the inner surface of the peripheral edge of the glass plate, press the other glass plate to the glass plate on which the spacer is molded, and form a hollow layer between the two glass plates A method for producing a double-glazed glass, characterized in that the glass plates are arranged to face each other at a predetermined interval through the spacer provided on the peripheral edge of the glass plate. In a resin composition having hot-melt adhesiveness, comprising an isobutylene polymer (A) having an alkenyl group at the terminal, a thermoplastic resin (B), and a compound (C) having at least two hydrosilyl groups in the molecule A spacer having a predetermined shape is formed, the spacer is bonded onto the inner surface of the peripheral edge of the glass plate, another glass plate is pressure-bonded to the glass plate to which the spacer is bonded, and both glass plates are placed between them. A method for producing a double-glazed glass, characterized in that the glass layers are arranged to face each other at a predetermined interval via the spacer provided on the peripheral edge of the glass plate so as to form a hollow layer.

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