JP2008201931A - Resin composition - Google Patents

Abstract

<P>PROBLEM TO BE SOLVED: To provide a resin composition that is excellent in gas-barrier properties, mechanical strengths and elasticity, exhibits low gravitational deformation even under a high temperature condition and has good hot-melt coatability. <P>SOLUTION: The composition comprises an isobutylene polymer (A) and an isobutylene diblock copolymer (B) comprised of a polymer block composed of an aromatic vinyl compound as its constituting monomer and polymer block composed of isobutylene as its constituting monomer, where the weight ratio of the polymer block composed of isobutylene as its constituting monomer to the polymer block composed of an aromatic vinyl compound as its constituting monomer is such that (the polymer block composed of isobutylene as its constituting monomer)/(the polymer block composed of an aromatic vinyl compound as its constituting monomer) is 60/40 to 20/80. <P>COPYRIGHT: (C)2008,JPO&INPIT

Description

  The present invention relates to a resin composition that is excellent in gas barrier properties, mechanical strength and elasticity, and further exhibits low self-weight deformation property and hot melt coating property even under high temperature conditions. The present invention also relates to a sealing material comprising such a resin composition, in particular, a hot-melt sealing material for multi-layer glass and a hot-melt spacer for multi-layer glass.

  Sealing materials are widely used in automobiles and building materials as materials that are filled in joints in order to obtain water tightness and air tightness. Sealing materials are required to have high airtightness, and other required characteristics differ depending on the application used, but high elasticity and high mechanical strength are required in many applications.

One example of the use of the sealing material for building materials is a double-layer glass. Multi-layer glass is generally composed of two or more glass panels, and a spacer is interposed between them to maintain a space. In double-glazed glass, a sealant is applied between the spacer and the glass, and the space between the glass panels is filled with a gas such as dry air, nitrogen, argon, or sulfur hexafluoride. Effects such as properties and prevention of condensation can be obtained.
There are various structures of the double-glazed glass, and various sealing materials are applied by various methods according to the structure. Examples of such a sealing material include a hot melt adhesive and a hot melt spacer. As an example of a double-layer glass using a hot-melt material, a material obtained by kneading a desiccant into a thermoplastic resin such as hot-melt butyl composed mainly of a vinyl chloride resin or an isobutylene polymer is used as a spacer. Multi-layer glass is known (Patent Document 1).
Hot melt butyl composed mainly of this isobutylene polymer is often used as a sealing material for multi-layer glass because of its properties such as gas barrier properties, weather resistance, and adhesiveness that can maintain airtightness and watertightness. Material. Specifically, in the case of a double-glazed glass structure that uses an aluminum spacer with a desiccant inside, it can be used as a primary sealant for fixing between the aluminum spacer and the glass by hot-melt coating. In addition, hot melt coating as a secondary sealant is applied to the outside of the aluminum spacer, and recently, a material obtained by kneading a desiccant into this hot melt butyl is hot melt applied to the end of one side of the multi-layer glass as a thermoplastic. Used as a resin spacer. In any configuration, the role that hot melt butyl should play is to maintain hermeticity by adhesion to glass, and it is required that it does not break or deform during long-term use. In some cases, the airtightness is lost due to the inability to maintain the performance. In particular, deformation due to its own weight under high-temperature conditions (self-weight deformability) and lack of elasticity and mechanical strength under high-temperature conditions may be problematic.
A method of adding a styrene / isobutylene-based thermoplastic elastomer to hot melt butyl is known for the purpose of improving its own weight deformability under high temperature conditions and lack of elasticity and mechanical strength under high temperature conditions. .
Examples of using styrenic thermoplastic elastomer include elastic sealing material using styrene / isobutylene triblock polymer and star block copolymer (Patent Document 2), styrene / isobutylene triblock copolymer and diblock. A sealing material for multilayer glass using a copolymer (Patent Document 3) may be mentioned. Among such styrene / isobutylene block copolymers, when a triblock or star block is used, the self-weight deformability under high temperature conditions is improved, but the hot melt coatability may be insufficient. In addition, when a diblock copolymer is used, even if a block body having a low styrene content is added, the self-weight deformation property under high temperature conditions may not be improved.
Therefore, there has been a demand for a material having a good hot melt coating property while improving the self-weight deformation property of hot melt butyl under high temperature conditions.
Japanese Unexamined Patent Publication No. 7-17748 JP 2003-506557 A JP 2006-273682 A

  An object of the present invention is a resin composition that can be used as a sealing material, particularly a hot-melt sealing material for double-glazed glass and a hot-melt spacer for double-glazed glass, and has excellent gas barrier properties, mechanical strength, and elasticity. Another object of the present invention is to provide a resin composition exhibiting low self-weight deformability and good hot melt coating property even under high temperature conditions.

As a result of intensive studies, the present inventors have completed the present invention.
That is, the present invention comprises an isobutylene polymer (A), a polymer block containing an aromatic vinyl compound as a constituent monomer, and a polymer block containing isobutylene as a constituent monomer, and isobutylene is a constituent monomer. The weight ratio of the polymer block comprising a polymer and the polymer block comprising an aromatic vinyl compound as a constituent monomer is (polymer block comprising isobutylene as a constituent monomer) / (unit comprising an aromatic vinyl compound). It relates to a resin composition comprising an isobutylene-based diblock copolymer (B) wherein the polymer block is a polymer) = 60/40 to 20/80.
As a preferable embodiment, the present invention relates to a resin composition in which the number average molecular weight of the isobutylene diblock copolymer (B) is 20,000 to 70,000.

As a preferred embodiment, the present invention relates to a resin composition characterized in that the resin composition further contains a filler (C).
As a preferred embodiment, the present invention relates to a resin composition characterized in that the filler (C) is carbon black.

  As a preferred embodiment, the present invention relates to a resin composition characterized in that the resin composition further contains a hygroscopic compound (D).

  A preferred embodiment relates to a resin composition, wherein the hygroscopic compound (D) is at least one selected from the group consisting of silica gel, alumina and zeolite.

  Furthermore, this invention relates to the sealing material which consists of the said resin composition.

  Furthermore, this invention relates to the hot-melt-sealing material for multilayer glass which consists of the said resin composition.

  Furthermore, this invention relates to the hot-melt spacer for multilayer glass which consists of the said resin composition.

The resin composition according to the present invention exhibits low self-weight deformation even under high temperature conditions, and has high elasticity and mechanical strength as compared with conventional compositions, and also has good hot melt application. Excellent in gas barrier properties. Therefore, the resin composition according to the present invention is suitably used as a sealing material that requires high elasticity, mechanical strength, gas barrier and the like, particularly as a hot-melt sealing material for multi-layer glass and a hot-melt spacer for multi-layer glass. be able to.

The resin composition according to the present invention comprises an isobutylene polymer (A), a polymer block comprising an aromatic vinyl compound as a constituent monomer, and a polymer block comprising isobutylene as a constituent monomer. It consists of a diblock copolymer (B).
In the composition according to the present invention, hot melt adhesiveness is imparted by the isobutylene polymer (A). The isobutylene block polymer (B) has high gas barrier properties derived from having an isobutylene block and rigidity derived from having an aromatic vinyl compound block. Compared to the case where other thermoplastic elastomers are used, there is an advantage that the water-tightness and air-tightness of the composition are not impaired, and it is difficult to be deformed by its own weight under high-temperature conditions. Furthermore, rigidity is provided by the filler (C).

  The isobutylene polymer (A) corresponds to many products that are usually marketed as polyisobutylene, polybutene, and the like. Specifically, EXEXON Vistanex (LM-MS, MH, H or MML-80, 100, 120, 140, etc.) ), Nippon Petroleum Tetrax (3T, 4T, 5T, 6T, etc.), Polybutene (HV) High Mall (4H, 5H, 6H, etc.), and BASF Opanol (B10, B12, B15, B50, B80, B100, B120, B150, B220, etc.).

  The isobutylene polymer (A) is not particularly limited, but the polymer preferably has 50 parts by weight or more, more preferably 80 parts by weight or more, still more preferably 90 parts by weight or more as a constituent monomer. To do.

  The monomer other than isobutylene contained 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. And 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-chloro Styrene, 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.
The number average molecular weight of the isobutylene polymer (A) is not particularly limited, but is preferably 1000 to 300,000, particularly preferably 10,000 to 100,000.
As the isobutylene polymer (A), those having various functional groups in the molecular chain or at the molecular chain terminal can be used for the purpose of improving the adhesiveness / adhesiveness of the composition of the present invention to the glass plate. . Examples of the functional group include ether groups such as epoxy groups, hydroxyl groups, amino groups, alkylamino groups, and alkoxyl groups, ester groups such as carboxyl groups, alkoxycarbonyl groups, and acyloxyl groups, carbamoyl groups, alkylcarbamoyl groups, and acylamino groups. Amide groups, acid anhydride groups such as maleic anhydride, silyl groups, allyl groups, vinyl groups, and the like. The isobutylene polymer (A) may have only one kind of these functional groups, or may have two or more kinds. Preferred functional groups include epoxy groups, amino groups, ether groups, ester groups, amide groups, silyl groups, allyl groups, and vinyl groups.

Although it does not specifically limit as an aromatic vinyl type compound which comprises an isobutylene type diblock copolymer (B), For example, what was illustrated by the aromatic vinyl mentioned above etc. are mentioned.
The polymer block containing an aromatic vinyl compound as a constituent monomer 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 occupies 60% by weight or more in the entire polymer block, and more preferably 80% by weight or more. When the aromatic vinyl compound is 60% by weight or less in the entire polymer block, the cohesive force of the polymer block is lowered, which is not preferable. The monomer other than the aromatic vinyl compound is not particularly limited as long as it is a monomer that can be cationically polymerized with the aromatic vinyl compound. For example, isobutylene, the above aliphatic olefins, dienes, vinyl ethers, β -Monomers such as pinene can be exemplified. These may be used alone or in combination of two or more.

The polymer block containing isobutylene as a constituent monomer may or may not contain a monomer other than isobutylene. When a monomer other than isobutylene is included, isobutylene preferably accounts for 60% by weight or more, and more preferably 80% by weight or more in the entire polymer block. The monomer other than isobutylene in the polymer block is not particularly limited as long as it is a monomer that can be cationically polymerized with isobutylene. For example, the aromatic vinyl, aliphatic olefins, dienes, vinyl ethers described above, Examples thereof include monomers such as β-pinene. These may be used alone or in combination of two or more.
The weight ratio of the polymer block having isobutylene as a constituent monomer and the polymer block having an aromatic vinyl compound as a constituent monomer in the composition of the isobutylene diblock copolymer (B) is not particularly limited. However, (polymer block having isobutylene as a constituent monomer) / (polymer block having an aromatic vinyl compound as a constituent monomer) = 60/40 to 20/80 is preferable. In particular, 60/40 to 40/60 is preferable because of its own weight deformability under high temperature conditions. When the ratio of the polymer block having an aromatic vinyl compound as a constituent monomer is too small, the self-weight deformability under high temperature conditions increases. Moreover, when the ratio becomes large, the gas barrier property of the resin composition may be impaired, or the function as a sealing material may be deteriorated, for example, the adhesive strength may be reduced.

  Although the number average molecular weight of an isobutylene type diblock copolymer (B) does not have a restriction | limiting in particular, 20000-70000 are preferable. In particular, from 30000 to 50000 is preferable from the viewpoint of its own weight deformability and hot melt coating property under high temperature conditions. When the molecular weight is too low, the self-weight deformability under high temperature conditions increases, and when the molecular weight is too large, the melt viscosity increases and the hot melt coatability deteriorates. In addition, the number average molecular weight in this specification is calculated in terms of polystyrene by gel permeation chromatography.

  Although there is no restriction | limiting in particular as a ratio of the isobutylene type diblock copolymer (B) in the resin composition which concerns on this invention, Preferably it is 1-100 weight part with respect to 100 weight part of isobutylene type polymer (A). Yes, more preferably 5 to 20 parts by weight. If the proportion of the isobutylene-based diblock copolymer (B) is small, the self-weight deformability under high temperature conditions increases, and if the proportion is large, the gas barrier property of the resin composition is impaired or the adhesive strength decreases. In some cases, the function as a sealing material may deteriorate.

  As the isobutylene diblock copolymer (B), those having various functional groups in the molecular chain or at the molecular chain terminal are used for the purpose of improving the adhesiveness / adhesiveness of the composition of the present invention to the glass plate. be able to. 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 acyloxyl 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 isobutylene diblock copolymer (B) may have only one of these functional groups, or may have two or more. Preferred functional groups include epoxy groups, amino groups, ether groups, ester groups, amide groups, silyl groups, allyl groups, and vinyl groups.

The production method of the isobutylene-based polymer (A) and the isobutylene-based diblock copolymer (B) is not particularly limited, and a known polymerization method can be used, but a block copolymer having a controlled structure can be used. In order to obtain, it is preferable to polymerize the monomer component which has isobutylene as a main component in presence of the compound represented by following General formula (1). When producing the isobutylene diblock copolymer (B), a monomer component mainly composed of an aromatic vinyl compound is further polymerized.
(CR ¹ R ² X) nR ³ ... General formula (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 polymer (A) and the isobutylene diblock copolymer (B) are produced by polymerization, a Lewis acid catalyst can also be present. 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 and} other metal halides; Et ₂ AlCl, EtAlCl _{2 and} other organic metal halides can be suitably 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 polymer (A) and the isobutylene diblock copolymer (B), 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 polymer (A) and the isobutylene-based diblock copolymer (B) can be carried out in an organic solvent as necessary, and the organic solvent is not particularly limited unless it substantially inhibits cationic polymerization. It can be used without. 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 considered in consideration of the balance of the polymerization characteristics of the monomers constituting the isobutylene-based polymer (A) and the isobutylene-based diblock copolymer (B) according to the present invention and the solubility of the resulting polymer. Are used alone or in combination of two or more. 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.

  The composition according to the present invention may further contain a filler (C). The filler (C) has the effect of improving the rigidity of the resin composition of the present invention, has the effect of improving the shape maintaining property in the operating temperature range, and the effect of suppressing sagging during hot melt application. There is no restriction | limiting in particular as an inorganic filler (C), 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.

  Although the compounding quantity of a filler (C) does not have a restriction | limiting in particular, It is preferable to set it as 1-300 weight part with respect to 100 weight part of isobutylene polymer (A), More preferably, it is 50-150 weight part. .

  The composition according to the present invention may further contain a hygroscopic compound (D). Examples of the hygroscopic compound (D) include zeolite, silica gel, and alumina, and any of these can be used. You may use these in combination of 2 or more type. Such a hygroscopic compound can reduce the water vapor transmission rate of the resin composition according to the present invention and prevent the voids sandwiched between the glass plates of the multilayer glass from becoming clouded by moisture. In order to achieve such an object effectively, it is preferable that the compounding quantity of a hygroscopic compound (D) is 1-100 weight part with respect to 100 weight part of isobutylene-type polymer (A).

Further, the resin composition according to the present invention may further contain a tackifier, a plasticizer, an antioxidant, an ultraviolet absorber, a light stabilizer, a pigment, a surfactant, a flame retardant, etc., as long as the physical properties are not impaired. Can be blended. Known antiblocking agents, antistatic agents, colorants, inorganic or organic antibacterial agents, lubricants, and the like can also be blended.
The tackifier is a low-molecular resin having a number average molecular weight of 300 to 3000 and a softening point of 60 to 150 ° C. based on the ring and ball method defined in JIS K-2207, and includes rosin and rosin derivatives, polyterpene resins, Aromatic modified terpene resins and their hydrides, terpene phenol resins, coumarone and indene resins, aliphatic petroleum resins, alicyclic petroleum resins and their hydrides, aromatic petroleum resins and their hydrides, aliphatic aromas A low molecular weight polymer of a group copolymer petroleum resin, a dicyclopentadiene petroleum resin and a hydride thereof, styrene or substituted styrene is exemplified.
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 is compatible with the isobutylene block copolymer (A) in order to achieve such a purpose and prevent bleed out. It is desirable to add a plasticizer, and paraffinic process oil, liquid polybutene, liquid polyisobutylene, and the like are preferably used.
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 and phosphorus antioxidants are used as secondary antioxidants by decomposing peroxides. Examples of sulfur antioxidants include thiobis (β-naphthol) and thiobis (N-phenyl-β). -Naphthylamine), 2-mercaptobenzothiazole, 2-mercaptobenzimidazole, dodecyl mercaptan, dilauryl thiodipropionate, distearyl thiodipropionate, pentaerythritol tetralauryl thiopropionate, tetramethylthiuram monosulfide, tetramethyl Examples include thiuram disulfide, nickel dibutyldithiocarbamate, 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 Ite, di (nonylphenyl) pentaerythritol diphosphite, tris (1,3-distearoyloxyisopropyl) phosphite, 4,4'-isopropiodenbis (2-t-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 according to the present invention is not particularly limited, and for example, mechanical mixing using a roll, a Banbury mixer, a kneader, a melting kettle equipped with a stirrer, or a single or twin screw extruder. Can be used. At this time, you may heat as needed. Moreover, it can also use the method of making it a uniform solution and distilling a solvent off.
The kneading conditions may be at or above the temperature at which the isobutylene diblock copolymer (B) melts, and is preferably 260 ° C. or less.

  If necessary, the resin composition according to the present invention can be molded using a molding method and a molding apparatus generally employed for a thermoplastic resin composition, for example, extrusion molding, injection molding, press molding, blow molding. It can shape | mold by etc.

The resin composition obtained as described above has excellent gas barrier properties, high elasticity and mechanical strength, and hardly undergoes self-weight deformation under high temperature conditions. On the other hand, when applying to glass, that is, when an applicator such as an applicator is assumed, shearing force is generated and it flows easily. Therefore, sealing materials, especially hot-melt sealing materials for multilayer glass and multilayer glass, are used. It can be suitably used as a hot melt spacer.

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

[Contents of components described in Examples, etc.]
PIB: polyisobutylene (manufactured by BASF, trade name “Opanol B12”)
SIB1: Styrene-isobutylene diblock copolymer 1 (described in Production Example 1, molecular weight 50000, styrene block content 50%)
SIB2: Styrene-isobutylene diblock copolymer 2 (described in Production Example 2, molecular weight 40000, styrene block content 60%)
SIB3: Styrene-isobutylene diblock copolymer 3 (described in Production Example 3, molecular weight 40000, styrene block content 50%)
SIB4: Styrene-isobutylene diblock copolymer 4 (described in Production Example 4, molecular weight 20000, styrene block content 50%)
SIB5: Styrene-isobutylene diblock copolymer 5 (described in Production Example 5, molecular weight 40000, styrene block content 15%)
SIB6: Styrene-isobutylene diblock copolymer 6 (described in Production Example 6, molecular weight 40000, styrene block content 30%)
SIBS: Styrene-isobutylene-styrene triblock copolymer (described in Production Example 7, molecular weight 100000, styrene block content 30%)
Talc (Fuji Talc Kogyo Co., Ltd., trade name “Talc LMR”)
Carbon black (trade name “Asahi Carbon # 60HN” manufactured by Asahi Carbon Co., Ltd.)
Zeolite (Molecular Sieves 3A)

Labo Plast Mill (Toyo Seiki Seisakusho Co., Ltd.): Batch type twin screw kneader

[Various test methods]
[Self-weight deformation under high temperature conditions / heat sag test]
First, the obtained resin composition was molded into a sheet having a width of 20 mm, a length of 30 mm, and a thickness of 4 mm using a mold and a press molding machine (set temperature: 180 ° C.). A glass plate having a width of 50 mm, a length of 50 mm, and a thickness of 5 mm was prepared, and the sheet was pressure-bonded perpendicularly to the glass surface as shown in FIG. The glass plate to which the sheet was pressure-bonded was fixed perpendicularly to the ground using a table and left in a hot air dryer at 90 ° C. for 2 hours. After the test for 2 hours, as shown in FIG. 2, the distance x (mm) between the original position and the heated position was measured for the lower position of the sheet. The self-weight deformability was evaluated by the size of the distance x (mm) after the heating test.
○: The distance x (mm) after the heating test is 1 mm or less.
Δ: Distance x (mm) after the heating test is greater than 1 mm and 3 mm or less.
X: Distance x (mm) after the heating test is larger than 3 mm.
[Mechanical strength / tensile strength at high temperature and room temperature]
In accordance with JIS K 6251, the test piece used was a 2 mm thick sheet punched with a No. 7 dumbbell. The tensile strength was 100 mm / min, and the tensile strength at 20% elongation was measured at 23 ° C. and 100 ° C., respectively.
[Gas barrier properties / moisture permeability]
The obtained composition was heated and pressed under the condition of 180 ° C. to produce a 0.9 mm thick sheet. The produced sheet was measured for moisture permeability of the composition at 40 ° C. and 90% RH according to JIS Z 0208.
◯: The measured moisture permeability is less than 1 g / m ² · day.
X: The measured value of moisture permeability is 1 g / m ² · day or more.
[Hot melt applicability]
[Wetting test]
The wettability of the resin composition with respect to the glass surface was evaluated under a temperature condition of 130 ° C. The detailed evaluation method is shown below. Place a resin composition sheet (2 mm thick, 3 cm x 3 cm) in a 130 ° C oven for 30 minutes on a glass plate (5 cm x 3 cm) so that air bubbles do not enter with a 2 kg roller. Lamination and the wettability of the glass surface and the resin composition sheet were visually observed.
○: There is no air bubble at the interface between the glass and the resin composition sheet.
X: Air bubbles are present at the interface between the glass and the resin composition sheet.
[Melt viscosity]
The melt viscosity of the obtained composition was measured according to JIS K 7199 at 130 ° C. and a capillary diameter of 2 mmφ at an apparent shear rate of 0.76 sec ⁻¹ .

(Production Example 1) [Production of SIB1]
After the inside of the polymerization vessel of the 2 L separable flask was purged with nitrogen, 300 mL of n-hexane (dried with molecular sieves) and 432 mL of butyl chloride (dried with molecular sieves) were added using a syringe. After cooling in a dry ice / methanol bath at −70 ° C., a Teflon (registered trademark) liquid feeding tube was connected to a pressure-resistant glass liquefied collection tube with a three-way cock containing 177 mL (1873 mmol) of isobutylene monomer, and polymerization was performed. Isobutylene monomer was fed into the container by nitrogen pressure. 0.65 g (4.2 mmol) of cumyl chloride and 0.94 g (10.8 mmol) of N, N-dimethylacetamide were added. Next, 6.6 mL (61 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, 117 g (1121 mmol) of styrene monomer was added into 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 desired isobutylene diblock copolymer. In addition, the number average molecular weight of the isobutylene polymer before styrene addition was 25000, and the number average molecular weight of the block copolymer after styrene polymerization was 50000. The styrene block content in the block copolymer was 50% by weight.
(Production Examples 2 to 6) [Production of SIB 2 to 6]
In the same manner as in Production Example 1, the amounts of isobutylene monomer and styrene monomer were changed to obtain an isobutylene diblock copolymer. The number average molecular weight of each block copolymer and the styrene block content in the block copolymer are shown in Tables 1 and 2. Here, when forming a polymer block containing isobutylene as a constituent monomer, only an isobutylene monomer was added, and when forming a polymer block containing styrene as a constituent monomer, only a styrene monomer was added.
(Production Example 7) [Production of SIBS]
After the inside of the polymerization vessel of the 2 L separable flask was purged with nitrogen, 300 mL of n-hexane (dried with molecular sieves) and 432 mL of butyl chloride (dried with molecular sieves) were added using a syringe. After cooling in a dry ice / methanol bath at −70 ° C., a Teflon (registered trademark) liquid feeding tube was connected to a pressure-resistant glass liquefied sampling tube with a three-way cock containing 184 mL (1942 mmol) of isobutylene monomer, and polymerization was performed. Isobutylene monomer was fed into the container by nitrogen pressure. 0.36 g (1.6 mmol) of p-dicumyl chloride and 0.94 g (10.8 mmol) of N, N-dimethylacetamide were added. Next, 2.1 mL (18.7 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, 51 g (488 mmol) of styrene monomer was added into 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. In addition, the number average molecular weight of the isobutylene polymer before styrene addition was 70000, and the number average molecular weight of the block copolymer after styrene polymerization was 100,000. The styrene block content was 30%.
(Example 1)
10 parts by weight of SIB1 / 35 parts by weight of PIB / 15 parts by weight of carbon black / 25 parts by weight of talc / 15 parts by weight of zeolite are melt-kneaded in a lab plast mill at a temperature of 170 ° C. for 10 minutes to obtain a resin composition. It was. Using this composition, various physical properties were evaluated by the above methods. The results are shown in Table 1.
(Examples 2 to 4)
As shown in Table 1, a resin composition was obtained in the same manner as in Example 1 except that the type of the isobutylene diblock copolymer (B) was changed. Using this composition, various physical properties were evaluated by the above methods.
(Comparative Example 1)
45 parts by weight of PIB / 15 parts by weight of carbon black / 25 parts by weight of talc / 15 parts by weight of zeolite were melt-kneaded for 10 minutes at 170 ° C. in a lab plast mill to obtain a resin composition. Using this composition, various physical properties were evaluated by the above methods. The results are shown in Table 2.
(Comparative Example 2)
45 parts by weight of PIB / 25 parts by weight of carbon black / 15 parts by weight of talc / 15 parts by weight of zeolite were melt-kneaded for 10 minutes at 170 ° C. in a lab plast mill to obtain a resin composition. Using this composition, various physical properties were evaluated by the above methods. The results are shown in Table 2.
(Comparative Example 3)
10 parts by weight of SIBS / 35 parts by weight of PIB / 15 parts by weight of carbon black / 25 parts by weight of talc / 15 parts by weight of zeolite are melt-kneaded in a lab plast mill at a temperature of 170 ° C. for 10 minutes to obtain a resin composition. It was. Using this composition, various physical properties were evaluated by the above methods. The results are shown in Table 2.
(Comparative Example 4)
10 parts by weight of SIB5 / 35 parts by weight of PIB / 15 parts by weight of carbon black / 25 parts by weight of talc / 15 parts by weight of zeolite are melt-kneaded in a lab plast mill at a temperature of 170 ° C. for 10 minutes to obtain a resin composition. It was. Using this composition, various physical properties were evaluated by the above methods. The results are shown in Table 2.
(Comparative Example 5)
10 parts by weight of SIB6 / 35 parts by weight of PIB / 15 parts by weight of carbon black / 25 parts by weight of talc / 15 parts by weight of zeolite are melt-kneaded in a lab plast mill at a temperature of 170 ° C. for 10 minutes to obtain a resin composition. It was. Using this composition, various physical properties were evaluated by the above methods. The results are shown in Table 2.

実施例１〜４は、ブロック体としてスチレン含量が４０％以上のジブロック体（ＳＩＢ）を添加することにより、高温条件下での自重変形性に優れ、ぬれ性が良好かつ溶融粘度も比較的低く、ホットメルト塗布性にも優れた樹脂組成物となる。また、高温および室温条件下での機械強度について、特に、高温条件下（１００℃）での引張強度が高い。

In Examples 1 to 4, by adding a diblock body (SIB) having a styrene content of 40% or more as a block body, it is excellent in its own weight deformability under high temperature conditions, has good wettability, and has a relatively high melt viscosity. The resin composition is low and excellent in hot melt coating property. Further, the mechanical strength under high temperature and room temperature conditions is particularly high in tensile strength under high temperature conditions (100 ° C.).

  On the other hand, Comparative Example 1 in which no block is added has poor self-weight deformability under high temperature conditions, and Comparative Example 2 in which the amount of carbon black is further increased is poor in self-weight deformability under high temperature conditions and has wettability. It deteriorates and the melt viscosity becomes relatively high, and the hot melt coating property is poor.

  In Comparative Example 3, triblock SIBS was added as a block body, but the self-weight deformation property and mechanical strength under high temperature conditions were improved, but the wettability was deteriorated and the melt viscosity was relatively high. Poor applicability.

  In Comparative Examples 4 and 5, SIB which is a diblock body having a relatively low styrene content (30% or less) was added as a block body, but the wettability was good and the melt viscosity was relatively low. As a result, its own weight deformation was poor.

  From the above, it has been found that the composition according to the present invention is excellent in both its own weight deformation property and hot melt coating property at high temperature. This resin composition can be suitably used as a sealing material, particularly a hot-melt sealing material for double-glazed glass and a hot-melt spacer for double-glazing.

The schematic block diagram of the test body for a self-weight deformability test. Sectional drawing of the test body of FIG.

Claims (9)

  A polymer comprising an isobutylene polymer (A), a polymer block comprising an aromatic vinyl compound as a constituent monomer, and a polymer block comprising isobutylene as a constituent monomer, wherein the polymer comprises isobutylene as a constituent monomer. The weight ratio of the polymer block containing the block and the aromatic vinyl compound as the constituent monomer is (polymer block containing isobutylene as the constituent monomer) / (weight containing the aromatic vinyl compound as the constituent monomer). Resin composition comprising an isobutylene diblock copolymer (B) in which the combined block) = 60/40 to 20/80. The resin composition according to claim 1, wherein the number average molecular weight of the isobutylene diblock copolymer (B) is 20,000 to 70,000.   The resin composition according to claim 1, wherein the resin composition further contains a filler (C).   The resin composition according to claim 3, wherein the filler (C) is carbon black.   The resin composition according to any one of claims 1 to 4, wherein the resin composition further contains a hygroscopic compound (D).   The resin composition according to claim 5, wherein the hygroscopic compound (D) is at least one selected from the group consisting of silica gel, alumina and zeolite.   The sealing material which consists of a resin composition in any one of Claims 1-6.   A hot-melt sealing material for multilayer glass, comprising the resin composition according to claim 1.   The hot-melt spacer for multilayer glass which consists of a resin composition in any one of Claims 1-6.

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