JP2019023153A - Intermediate film for laminated glass and laminated glass - Google Patents

Abstract

To provide an intermediate film for laminated glass which can effectively enhance sound insulation property of laminated glass.SOLUTION: An intermediate film for laminated glass has a first layer containing a thermoplastic resin and a plasticizer, and a second layer containing a thermoplastic resin and a plasticizer, where the second layer is arranged on a first surface side of the first layer, and a combination of the thermoplastic resin in the second layer and the plasticizer in the first layer is a combination in which the thermoplastic resin and the plasticize are not completely dissolved at 180°C in a liquid obtained mixing 8 pts.wt. of the thermoplastic resin in the second layer in 100 pts.wt. of the plasticizer in the first layer, or a combination in which cloudiness is not generated at 180°C and the cloudiness is generated at 130°C or higher when the temperature is reduced from 180°C, in the liquid obtained mixing 8 pts.wt. of the thermoplastic resin in the second layer in 100 pts.wt. of the plasticizer in the first layer.SELECTED DRAWING: Figure 1

Description

  The present invention relates to an interlayer film for laminated glass used for obtaining laminated glass. Moreover, this invention relates to the laminated glass using the said intermediate film for laminated glasses.

  In general, laminated glass is excellent in safety because the amount of glass fragments scattered is small even if it is damaged by an external impact. For this reason, the said laminated glass is widely used for a motor vehicle, a rail vehicle, an aircraft, a ship, a building, etc. The laminated glass is manufactured by sandwiching an interlayer film for laminated glass between a pair of glass plates.

  Examples of the interlayer film for laminated glass include a single-layer interlayer film having a single-layer structure and a multilayer interlayer film having a structure of two or more layers.

  Patent Document 1 below discloses a laminate (intermediate film) in which a sound insulation layer is located between at least two adhesive layers. The laminated glass is sandwiched between 2 mm thick glasses and pressed for 60 minutes under the conditions of a temperature of 140 ° C. and a pressure of 1 MPa. The loss coefficient α at 2000 Hz is 0.2 or more. About the laminated glass after holding this laminated glass at 18 ° C. for 1 month, the ratio β / α of the loss coefficient β to the loss coefficient α at 20 ° C. and 2000 Hz measured by a damping test by the central vibration method is 0.70 or more. It is. The sound insulation layer may contain an elastomer. The sound insulation layer does not contain a plasticizer.

  Patent Document 2 below discloses an intermediate film in which a layer containing polyvinyl acetal and a layer containing polyolefin are laminated.

JP, 2006-108225, A WO2011 / 016494A1

  As described in Patent Documents 1 and 2, an interlayer film including a layer using a thermoplastic component other than a polyvinyl acetal resin is known. However, the laminated glass using this interlayer film may not have a sufficiently high sound insulation property.

  The objective of this invention is providing the intermediate film for laminated glasses which can improve the sound-insulating property of a laminated glass effectively. Another object of the present invention is to provide a laminated glass using the interlayer film for laminated glass.

  According to a wide aspect of the present invention, a first layer including a thermoplastic resin and a plasticizer, and a second layer including a thermoplastic resin and a plasticizer, the first layer of the first layer is provided. The second layer is arranged on the surface side, and the combination of the thermoplastic resin in the second layer and the plasticizer in the first layer is the combination of the thermoplastic resin in the first layer. A combination of 100 parts by weight of a plasticizer mixed with 8 parts by weight of the thermoplastic resin in the second layer that does not completely dissolve at 180 ° C., or the plastic in the first layer. In a liquid in which 100 parts by weight of the agent was mixed with 8 parts by weight of the thermoplastic resin in the second layer, no fogging occurred at 180 ° C. and when the temperature was lowered from 180 ° C., the liquid was clouded at 130 ° C. Provided an interlayer film for laminated glass (hereinafter sometimes referred to as an interlayer film) It is.

  In a specific aspect of the intermediate film according to the present invention, a combination of the thermoplastic resin in the first layer and the plasticizer in the second layer is the plasticizer in the second layer. The combination of 100 parts by weight of the thermoplastic resin in the first layer mixed with 8 parts by weight of the thermoplastic resin does not completely dissolve at 180 ° C., or the plasticizer 100 in the second layer. In a liquid in which 8 parts by weight of the thermoplastic resin in the first layer is mixed with parts by weight, cloudiness does not occur at 180 ° C., and clouding occurs at 50 ° C. or more when the temperature is lowered from 180 ° C. It is a combination.

  On the specific situation with the intermediate film which concerns on this invention, the said thermoplastic resin in a said 1st layer is a thermoplastic elastomer.

  On the specific situation with the intermediate film which concerns on this invention, the said thermoplastic elastomer is aliphatic polyolefin.

  On the specific situation with the intermediate film which concerns on this invention, the said aliphatic polyolefin is a saturated aliphatic polyolefin.

  On the specific situation with the intermediate film which concerns on this invention, the said plasticizer in a said 1st layer is plasticizers other than an organic ester plasticizer.

  On the specific situation with the intermediate film which concerns on this invention, the said plasticizer in a said 1st layer is paraffin oil.

  In a specific aspect of the intermediate film according to the present invention, the thermoplastic resin in the second layer is a polyvinyl acetal resin.

  On the specific situation with the intermediate film which concerns on this invention, the said intermediate film is provided with the 3rd layer containing a thermoplastic resin and a plasticizer, and the 1st surface side opposite to the 1st surface side of the said 1st layer. The third layer is disposed on the surface side of 2, and the combination of the thermoplastic resin in the third layer and the plasticizer in the first layer is the same as in the first layer. A combination of 100 parts by weight of the plasticizer mixed with 8 parts by weight of the thermoplastic resin in the third layer does not completely dissolve at 180 ° C., or the combination in the first layer. In a liquid in which 100 parts by weight of a plasticizer is mixed with 8 parts by weight of the thermoplastic resin in the third layer, no fogging occurs at 180 ° C. and the temperature of the liquid is reduced from 180 ° C. to 130 ° C. or higher. It is a combination that causes cloudiness.

  In a specific aspect of the intermediate film according to the present invention, a combination of the thermoplastic resin in the first layer and the plasticizer in the third layer is the plasticizer in the third layer. A combination of 100 parts by weight of the thermoplastic resin in the first layer mixed with 8 parts by weight of the thermoplastic resin that does not completely dissolve at 180 ° C., or the plasticizer 100 in the third layer. In a liquid in which 8 parts by weight of the thermoplastic resin in the first layer is mixed with parts by weight, cloudiness does not occur at 180 ° C., and clouding occurs at 50 ° C. or more when the temperature is lowered from 180 ° C. It is a combination.

  On the specific situation with the intermediate film which concerns on this invention, the said thermoplastic resin in a said 3rd layer is polyvinyl acetal resin.

  According to a wide aspect of the present invention, the first laminated glass member, the second laminated glass member, and the interlayer film for laminated glass described above are provided, and the first laminated glass member and the second laminated glass are provided. There is provided a laminated glass in which the interlayer film for laminated glass is disposed between the members.

  The interlayer film for laminated glass according to the present invention includes a first layer containing a thermoplastic resin and a plasticizer, and a second layer containing a thermoplastic resin and a plasticizer. In the interlayer film for laminated glass according to the present invention, the second layer is disposed on the first surface side of the first layer. In the interlayer film for laminated glass according to the present invention, a combination of the thermoplastic resin in the second layer and the plasticizer in the first layer is 100 weights of the plasticizer in the first layer. A liquid in which 8 parts by weight of the thermoplastic resin in the second layer is mixed with a part shows a combination exhibiting specific properties. Since the interlayer film for laminated glass according to the present invention has the above-described configuration, the sound insulation of the laminated glass can be effectively improved.

FIG. 1 is a cross-sectional view schematically showing an interlayer film for laminated glass according to the first embodiment of the present invention. FIG. 2 is a cross-sectional view schematically showing an example of a laminated glass using the laminated glass interlayer film shown in FIG.

  Hereinafter, the present invention will be described in detail.

(Interlayer film for laminated glass)
The interlayer film for laminated glass according to the present invention (hereinafter sometimes referred to as an interlayer film) includes a first layer and a second layer. The second layer is disposed on the first surface side of the first layer. The first layer includes a thermoplastic resin and a plasticizer. The first layer is a thermoplastic resin layer. The second layer includes a second layer containing a thermoplastic resin and a plasticizer. The intermediate film which concerns on this invention is equipped with the thermoplastic resin layer (1st layer) containing a thermoplastic resin as thermoplastic resins other than polyvinyl acetal resin.

  In the interlayer film according to the present invention, the combination of the thermoplastic resin in the second layer and the plasticizer in the first layer satisfies the following first configuration or the following second configuration. It is a combination to do.

First configuration: 100 parts by weight of the plasticizer in the first layer and 8 parts by weight of the thermoplastic resin in the second layer are not completely dissolved at 180 ° C. Structure: 100 parts by weight of the plasticizer in the first layer and 8 parts by weight of the thermoplastic resin in the second layer were mixed, and no fogging occurred at 180 ° C., and the liquid was removed from 180 ° C. Cloudiness occurs above 130 ° C when the temperature is lowered

  In the present invention, since the above-described configuration is provided, in the intermediate film including a layer using a thermoplastic component other than the polyvinyl acetal resin, the sound insulating property of the laminated glass including the intermediate film can be effectively increased. .

  When producing laminated glass, heat treatment is performed by an autoclave or the like. In a general multilayer interlayer film, when heated, the plasticizer moves between the layers, and the distribution of the plasticizer changes. For this reason, in the conventional multilayer intermediate film, the sound insulation of the laminated glass immediately after production may be low.

  In the present invention, since the plasticizer hardly migrates, the sound insulating property of the laminated glass can be improved even immediately after the production. Furthermore, when time elapses immediately after fabrication, a change in sound insulation of the laminated glass can be suppressed. When the first configuration or the second configuration is satisfied, the compatibility between the thermoplastic resin in the second layer and the plasticizer in the first layer is considerably low. For this reason, for example, the plasticizer in the first layer is unlikely to move to the second layer. For this reason, the layer using the thermoplastic component other than the polyvinyl acetal resin can sufficiently exhibit the effect of improving the sound insulation of the laminated glass. The intermediate film may satisfy the first configuration or the second configuration. The intermediate film preferably satisfies the first configuration.

  From the viewpoint of further improving sound insulation, in the intermediate film according to the present invention, the combination of the thermoplastic resin in the third layer and the plasticizer in the first layer is the following 1A: It is preferable that the configuration or a combination satisfying the following configuration 2A is satisfied. In this case, as a result of the plasticizer in the first layer becoming difficult to move to the third layer, sound insulation is effectively enhanced. The intermediate film may satisfy the following 1A configuration or may satisfy the following 2A configuration. The intermediate film preferably satisfies the following configuration 1A.

1A configuration: 100 parts by weight of the plasticizer in the first layer and 8 parts by weight of the thermoplastic resin in the third layer are not completely dissolved at 180 ° C. Structure: 100 parts by weight of the plasticizer in the first layer and 8 parts by weight of the thermoplastic resin in the third layer were mixed with no fog at 180 ° C., and the liquid was removed from 180 ° C. Cloudiness occurs above 130 ° C when the temperature is lowered

  From the viewpoint of further improving sound insulation, in the intermediate film according to the present invention, the combination of the thermoplastic resin in the first layer and the plasticizer in the second layer is the following third. It is preferable that the configuration or a combination satisfying the following fourth configuration is satisfied. In this case, as a result of the plasticizer in the second layer becoming difficult to move to the first layer, sound insulation is effectively enhanced. The intermediate film may satisfy the following third configuration, or may satisfy the following fourth configuration. The intermediate film preferably satisfies the following third configuration.

Third configuration: 100 parts by weight of the plasticizer in the second layer and 8 parts by weight of the thermoplastic resin in the first layer are not completely dissolved at 180 ° C. Constitution: 100 parts by weight of the plasticizer in the second layer and 8 parts by weight of the thermoplastic resin in the first layer are mixed with no fog at 180 ° C., and the liquid is removed from 180 ° C. Cloudiness occurs above 50 ° C when the temperature is lowered

  From the viewpoint of further improving sound insulation, in the intermediate film according to the present invention, the combination of the thermoplastic elastomer in the first layer and the plasticizer in the third layer is the following 3A: It is preferable that it is a combination that satisfies the configuration or the following configuration 4A. As a result of the plasticizer in the third layer becoming difficult to migrate to the first layer, the sound insulation is effectively increased. The intermediate film may satisfy the following 3A configuration, or may satisfy the following 4A configuration. The intermediate film preferably satisfies the following configuration 4A.

3A configuration: 100 A part by weight of the plasticizer in the third layer and 8 parts by weight of the thermoplastic resin in the first layer are not completely dissolved at 180 ° C. 4A configuration : 100 parts by weight of the plasticizer in the third layer was mixed with 8 parts by weight of the thermoplastic resin in the first layer, and no fogging occurred at 180 ° C. and the liquid was heated from 180 ° C. Cloudiness occurs above 50 ° C when reduced

  In the first, first, third, and third configurations, “not completely dissolved” means that a solution obtained by mixing 100 parts by weight of the plasticizer with 8 parts by weight of the thermoplastic resin is heated to 180 ° C. and stirred. Also means that the resin remains undissolved.

  In the second, second, fourth, and fourth configuration, the clouding temperature is the cloud point.

  From the viewpoint of effectively improving sound insulation, in the second configuration and the second A configuration, the cloud point is preferably 140 ° C. or higher, more preferably 150 ° C. or higher.

  From the viewpoint of effectively improving sound insulation, in the fourth configuration and the fourth configuration A, the cloud point is preferably 60 ° C. or higher, more preferably 70 ° C. or higher.

  The cloud point is a cloud point measured in accordance with JIS K2266 “Pour point of crude oil and petroleum products and cloud point test method of petroleum products”. Specifically, the cloud point measured using the thermoplastic resin and the plasticizer is measured as follows.

  3.5 g (100 parts by weight) of a plasticizer and 0.28 g (8 parts by weight) of a thermoplastic resin are prepared. In a test tube (2 cm in diameter), 3.5 g (100 parts by weight) of the plasticizer and 0.28 g (8 parts by weight) of the thermoplastic resin are mixed. A liquid in which the thermoplastic resin is mixed with the plasticizer is heated to 180 ° C. When the thermoplastic resin is not completely dissolved in the liquid heated to 180 ° C., the first, first, third, and third structures are provided. When the thermoplastic resin is completely dissolved in the liquid heated to 180 ° C., the temperature of the liquid is lowered to −15 ° C. by leaving the test tube in an atmosphere of −20 ° C. In the second, second, fourth, and fourth configuration, the cloud point means a temperature at which the liquid is clouded (first cloud point determination method). The higher the cloud point, the lower the compatibility between the thermoplastic resin and the plasticizer.

  Examples of methods for measuring the temperature at which the liquid is clouded (cloud point) include, for example, a method of visually observing the appearance of the liquid, a method of measuring the haze of the liquid with a haze meter, and a multi-stage limit sample regarding cloudiness in advance. A method of determining the fogging in comparison with the limit sample is prepared. A method of visually observing the appearance of the liquid is preferable. When measuring the haze of a liquid with a haze meter, let the temperature which becomes 10% or more of haze be a cloud point. In order to specify the temperature at which fogging occurs more accurately, the following measurement method may be used.

  3.5 g (100 parts by weight) of a plasticizer and 0.28 g (8 parts by weight) of a thermoplastic resin are prepared. In a test tube (2 cm in diameter), 3.5 g (100 parts by weight) of the plasticizer and 0.28 g (8 parts by weight) of the thermoplastic resin are mixed. A liquid in which the thermoplastic resin is mixed with the plasticizer is heated to 180 ° C. When the thermoplastic resin is not completely dissolved in the liquid heated to 180 ° C., the first, first, third, and third structures are provided. If the thermoplastic resin is completely dissolved in the liquid heated to 180 ° C., the liquid heated to 180 ° C. is left in a temperature-controlled room at a predetermined temperature for 1 hour. While maintaining the temperature of the temperature-controlled room, the haze of the liquid in the test tube is measured with a haze meter. In the second, second, fourth, and fourth configuration, the lowest storage temperature of the temperature-controlled room having a haze of 10% or more is defined as a cloud point (second cloud point determination method). For example, after each test tube is left in a temperature-controlled room at 155 ° C., 150 ° C., and 145 ° C. for 1 hour, the temperature of the temperature-controlled room is maintained and the haze of the liquid in the test tube is measured with a haze meter. By changing the storage temperature, the cloud point can be specifically identified.

  The content of the plasticizer in the first layer with respect to 100 parts by weight of the thermoplastic resin in the first layer after storing the intermediate film at 140 ° C. for 0.5 hour, and the intermediate film at 0.5 hours at 140 ° C. The difference between the content of the plasticizer in the first layer and the content of the plasticizer in the first layer relative to 100 parts by weight of the thermoplastic resin in the first layer after storage at 20 ° C. for 1 month is defined as content difference (1). The content difference (1) is preferably 0 part by weight or more, preferably 10 parts by weight or less, more preferably 7 parts by weight or less. In this case, the sound insulation is further enhanced.

  The content of the plasticizer in the second layer with respect to 100 parts by weight of the thermoplastic resin in the second layer after storing the intermediate film at 140 ° C. for 0.5 hour, and the intermediate film at 0.5 hours at 140 ° C. The difference between the content of the plasticizer in the second layer and the content of the plasticizer in the second layer with respect to 100 parts by weight of the thermoplastic resin in the second layer after storage for 0.5 hours at 20 ° C. and the content difference (2) To do. The content difference (2) is preferably 0 part by weight or more, preferably 2 parts by weight or less, more preferably 1 part by weight or less. In this case, the sound insulation is further enhanced.

  The content of the plasticizer in the third layer with respect to 100 parts by weight of the thermoplastic resin in the third layer after storing the intermediate film at 140 ° C. for 0.5 hour, and the intermediate film at 0.5 hours at 140 ° C. The difference between the content of the plasticizer in the third layer and the content of the plasticizer in the third layer with respect to 100 parts by weight of the thermoplastic resin in the third layer after storage for 0.5 hours at 20 ° C. and the content difference (3) To do. The content difference (3) is preferably 0 part by weight or more, preferably 2 parts by weight or less, more preferably 1 part by weight or less. In this case, the sound insulation is further enhanced.

  From the viewpoint of further enhancing the sound insulation, the glass transition temperature of the first layer exists in a temperature range of −10 ° C. to 10 ° C., and the temperature range of −10 ° C. to 10 ° C. of the first layer. It is preferable that the maximum value of tan δ is 1.5 or more. From the viewpoint of more effectively improving the sound insulation, the maximum value of tan δ of the first layer is preferably 2.0 or more, more preferably 2.5 or more.

  As a method of measuring the glass transition temperature and tan δ, the obtained interlayer film was stored for 12 hours in an environment of room temperature 23 ± 2 ° C. and humidity 25 ± 5%, and immediately after the “ARES-” manufactured by TA Instruments was used. The method of measuring viscoelasticity using G2 "is mentioned. Using a parallel plate with a diameter of 8 mm as a jig, the glass transition temperature and tan δ are measured under the conditions of decreasing the temperature from 30 ° C. to 100 ° C. at a temperature drop rate of 3 ° C./min, and under the conditions of frequency 1 Hz and strain 1%. It is preferable to do. For an intermediate film having a structure of two or more layers, the respective layers may be peeled and the glass transition temperature of the measurement target layer may be measured.

  The intermediate film according to the present invention has a structure of two or more layers. The interlayer film according to the present invention may have a two-layer structure or may have a three-layer structure or more.

  From the viewpoint of effectively improving sound insulation and adhesion between the glass and the interlayer film, the interlayer film according to the present invention is disposed on the first surface side of the first layer and the first layer side of the first layer. And a third layer arranged on the second surface side opposite to the first surface side of the first layer. The third layer preferably contains a thermoplastic resin and a plasticizer.

  From the viewpoint of effectively improving sound insulation and adhesion between the glass and the interlayer film, the first layer is preferably not a surface layer in the interlayer film, and is preferably an interlayer in the interlayer film. . However, the first layer may be a surface layer in the intermediate film.

  From the viewpoint of enhancing the transparency of the laminated glass, the visible light transmittance of the interlayer film is preferably 70% or more, more preferably 80% or more, and still more preferably 85% or more.

  The visible light transmittance is measured at a wavelength of 380 to 780 nm according to JIS R3211 (1998) using a spectrophotometer (“U-4100” manufactured by Hitachi High-Tech).

  The visible light transmittance of the intermediate film may be measured by disposing an intermediate film between two clear glasses.

  In order to increase the visible light transmittance, the intermediate film and the first layer may not contain a colorant and may not contain carbon black.

  Hereinafter, specific embodiments of the present invention will be described with reference to the drawings.

  FIG. 1 is a cross-sectional view schematically showing an interlayer film for laminated glass according to the first embodiment of the present invention.

  The intermediate film 11 shown in FIG. 1 is a multilayer intermediate film having a structure of two or more layers. The intermediate film 11 is used to obtain a laminated glass. The intermediate film 11 is an intermediate film for laminated glass. The intermediate film 11 includes a first layer 1, a second layer 2, and a third layer 3. On the first surface 1a side of the first layer 1, the second layer 2 is disposed and laminated. On the second surface 1b side opposite to the first surface 1a of the first layer 1, the third layer 3 is disposed and laminated. The first layer 1 is an intermediate layer. Each of the second layer 2 and the third layer 3 is a protective layer, and is a surface layer in the present embodiment. The first layer 1 is arranged between the second layer 2 and the third layer 3 and is sandwiched between them. Therefore, the intermediate film 11 has a multilayer structure (second layer 2 / first layer 1 / third layer) in which the second layer 2, the first layer 1, and the third layer 3 are laminated in this order. Having layer 3).

  In the intermediate film 11, the first layer 1 includes a thermoplastic resin and a plasticizer. The second layer 2 includes a thermoplastic resin and a plasticizer. The third layer 3 includes a thermoplastic resin and a plasticizer.

  Other layers may be disposed between the second layer 2 and the first layer 1 and between the first layer 1 and the third layer 3, respectively. The second layer 2 and the first layer 1 and the first layer 1 and the third layer 3 are preferably laminated directly. Examples of other layers include an adhesive layer and a layer containing polyethylene terephthalate.

  Hereinafter, details of the first layer, the second layer, and the third layer constituting the intermediate film according to the present invention, and the first layer, the second layer, and the third layer will be described. The details of each component contained in are described.

(Thermoplastic resin in the first layer)
The first layer includes a thermoplastic resin (hereinafter sometimes referred to as a thermoplastic resin (1)). As for the said thermoplastic resin, only 1 type may be used and 2 or more types may be used together.

  From the viewpoint of effectively improving sound insulation, the thermoplastic resin in the first layer is preferably a thermoplastic elastomer. The thermoplastic resin is a resin that softens when heated and exhibits plasticity and solidifies when cooled to room temperature. The thermoplastic elastomer means, among thermoplastic resins, a resin that softens when heated and exhibits plasticity, and solidifies when cooled to room temperature (25 ° C.) and exhibits rubber elasticity. The inventors of the present invention have studied to improve the sound insulating property of laminated glass in an intermediate film having a layer using a thermoplastic resin. As a result, the present inventors have found a configuration that can improve the sound insulation of the laminated glass.

  In addition, the present inventors have also studied to improve the sound insulation of the laminated glass even in an intermediate film including a layer using a thermoplastic component other than the polyvinyl acetal resin. As a result, the present inventors have found a configuration capable of enhancing the sound insulating properties of the laminated glass even in an intermediate film including a layer using a thermoplastic component other than the polyvinyl acetal resin.

  Examples of the thermoplastic resin (1) include aliphatic polyolefin, polystyrene, ethylene-vinyl acetate copolymer resin, ethylene-acrylic acid copolymer resin, polyurethane resin and polyvinyl alcohol resin, polyvinyl acetate resin, and polyester resin. Can be mentioned.

  The thermoplastic resin exemplified above can be made into a thermoplastic elastomer by adjusting the molecular structure and degree of polymerization of the resin. The thermoplastic elastomer is preferably an aliphatic polyolefin or a styrene elastomer, more preferably an aliphatic polyolefin from the viewpoint of effectively improving sound insulation.

  The aliphatic polyolefin may be a saturated aliphatic polyolefin or an unsaturated aliphatic polyolefin. The aliphatic polyolefin may be a polyolefin having a chain olefin as a monomer or a polyolefin having a cyclic olefin as a monomer. From the viewpoint of effectively enhancing the storage stability and sound insulation of the interlayer film, the aliphatic polyolefin is preferably a saturated aliphatic polyolefin.

  Examples of the aliphatic polyolefin material include ethylene, propylene, 1-butene, trans-2-butene, cis-2-butene, 1-pentene, trans-2-pentene, cis-2-pentene, 1-hexene and trans. 2-hexene, cis-2-hexene, trans-3-hexene, cis-3-hexene, 1-heptene, trans-2-heptene, cis-2-heptene, trans-3-heptene, cis-3-heptene 1-octene, trans-2-octene, cis-2-octene, trans-3-octene, cis-3-octene, trans-4-octene, cis-4-octene, 1-nonene, trans-2-nonene Cis-2-nonene, trans-3-nonene, cis-3-nonene, tran -4-nonene, cis-4-nonene, 1-decene, trans-2-decene, cis-2-decene, trans-3-decene, cis-3-decene, trans-4-decene, cis-4-decene , Trans-5-decene, cis-5-decene, 4-methyl-1-pentene, vinylcyclohexane and the like.

  From the viewpoint of effectively improving sound insulation, the aliphatic polyolefin preferably has a chain hydrocarbon group in the side chain.

  From the viewpoint of improving interlayer adhesion, the aliphatic polyolefin may be a modified aliphatic polyolefin. The modified aliphatic polyolefin preferably has a carboxyl group, a carboxylic anhydride group, a hydroxyl group or an epoxy group. The modified aliphatic polyolefin may have these groups in the side chain of the molecular chain or at the terminal.

(Thermoplastic resin in the second and third layers)
From the viewpoint of effectively increasing the adhesion between the glass and the interlayer film, the second layer includes a thermoplastic resin (hereinafter, may be referred to as a thermoplastic resin (2)), and the first layer It is preferable to include a thermoplastic resin other than the thermoplastic resin of the layer, and it is more preferable to include a polyvinyl acetal resin (hereinafter sometimes referred to as a polyvinyl acetal resin (2)). From the viewpoint of effectively increasing the adhesion between the glass and the interlayer film, the third layer preferably contains a thermoplastic resin (hereinafter sometimes referred to as a thermoplastic resin (3)). It is more preferable to include a thermoplastic resin other than the thermoplastic resin of the first layer, and it is even more preferable to include a polyvinyl acetal resin (hereinafter sometimes referred to as a polyvinyl acetal resin (3)).

  The thermoplastic resin (2) is selected in consideration of the first configuration and the second configuration.

  Examples of the thermoplastic resins (2) and (3) include polyvinyl acetal resins, ethylene-vinyl acetate copolymer resins, ethylene-acrylic acid copolymer resins, polyurethane resins, polyvinyl alcohol resins, polyvinyl acetate resins, and polyester resins. Etc. Thermoplastic resins other than these may be used.

  The polyvinyl acetal resin can be produced, for example, by acetalizing polyvinyl alcohol (PVA) with an aldehyde. The polyvinyl acetal resin is preferably an acetalized product of polyvinyl alcohol. The polyvinyl alcohol can be obtained, for example, by saponifying polyvinyl acetate. The degree of saponification of the polyvinyl alcohol is generally in the range of 70 to 99.9 mol%.

  The average degree of polymerization of the polyvinyl alcohol (PVA) is preferably 200 or more, more preferably 500 or more, still more preferably 1500 or more, still more preferably 1600 or more, preferably 5000 or less, more preferably 4000 or less, still more preferably. It is 3500 or less, particularly preferably 3000 or less. When the average degree of polymerization is not less than the above lower limit, the penetration resistance of the laminated glass is further enhanced. When the average degree of polymerization is not more than the above upper limit, the intermediate film can be easily molded.

  The average degree of polymerization of the polyvinyl alcohol is determined by a method based on JIS K6726 “Testing method for polyvinyl alcohol”.

  The number of carbon atoms of the acetal group contained in the polyvinyl acetal resin is not particularly limited. The aldehyde used when manufacturing the said polyvinyl acetal resin is not specifically limited. The number of carbon atoms of the acetal group in the polyvinyl acetal resin is preferably 3 to 5, and more preferably 3 or 4. When the carbon number of the acetal group in the polyvinyl acetal resin is 3 or more, the glass transition temperature of the intermediate film is sufficiently low.

  The aldehyde is not particularly limited. In general, aldehydes having 1 to 10 carbon atoms are preferably used. Examples of the aldehyde having 1 to 10 carbon atoms include formaldehyde, acetaldehyde, propionaldehyde, n-butyraldehyde, isobutyraldehyde, n-valeraldehyde, 2-ethylbutyraldehyde, n-hexylaldehyde, n-octylaldehyde, Examples include n-nonyl aldehyde, n-decyl aldehyde, formaldehyde, acetaldehyde, and benzaldehyde. Propionaldehyde, n-butyraldehyde, isobutyraldehyde, n-hexylaldehyde or n-valeraldehyde is preferred, propionaldehyde, n-butyraldehyde or isobutyraldehyde is more preferred, and n-butyraldehyde is still more preferred. As for the said aldehyde, only 1 type may be used and 2 or more types may be used together.

  The hydroxyl group content (hydroxyl group amount) of the polyvinyl acetal resin is preferably 15 mol% or more, more preferably 18 mol% or more, preferably 40 mol% or less, more preferably 35 mol% or less. When the hydroxyl group content is at least the above lower limit, the adhesive strength of the interlayer film is further increased. Further, when the hydroxyl group content is not more than the above upper limit, the flexibility of the interlayer film is increased, and the handling of the interlayer film is facilitated.

  The hydroxyl group content (hydroxyl content) of the polyvinyl acetal resin (1) is preferably 17 mol% or more, more preferably 20 mol% or more, still more preferably 22 mol% or more, preferably 28 mol% or less, more preferably. Is 27 mol% or less, more preferably 25 mol% or less, and particularly preferably 24 mol% or less. When the hydroxyl group content is equal to or higher than the lower limit, the mechanical strength of the interlayer film is further increased. In particular, when the hydroxyl group content of the polyvinyl acetal resin (1) is 20 mol% or more, the reaction efficiency is high and the productivity is excellent, and when it is 28 mol% or less, the sound insulation of the laminated glass is further enhanced. . Further, when the hydroxyl group content is not more than the above upper limit, the flexibility of the interlayer film is increased, and the handling of the interlayer film is facilitated.

  The content of each hydroxyl group in the polyvinyl acetal resin (2) and the polyvinyl acetal resin (3) is preferably 25 mol% or more, more preferably 28 mol% or more, more preferably 30 mol% or more, and still more preferably. 31.5 mol% or more, more preferably 32 mol% or more, particularly preferably 33 mol% or more, preferably 38 mol% or less, more preferably 37 mol% or less, still more preferably 36.5 mol% or less, particularly preferably Is 36 mol% or less. When the hydroxyl group content is at least the above lower limit, the adhesive strength of the interlayer film is further increased. Further, when the hydroxyl group content is not more than the above upper limit, the flexibility of the interlayer film is increased, and the handling of the interlayer film is facilitated.

  The hydroxyl group content of the polyvinyl acetal resin is a value indicating the mole fraction obtained by dividing the amount of ethylene groups to which the hydroxyl group is bonded by the total amount of ethylene groups in the main chain, as a percentage. The amount of ethylene group to which the hydroxyl group is bonded can be measured, for example, according to JIS K6728 “Testing method for polyvinyl butyral”.

  Each degree of acetylation of the polyvinyl acetal resin (2) and the polyvinyl acetal resin (3) is preferably 0.01 mol% or more, more preferably 0.5 mol% or more, preferably 10 mol% or less, more preferably. Is 2 mol% or less. When the acetylation degree is not less than the above lower limit, the compatibility between the polyvinyl acetal resin and the plasticizer is increased. When the acetylation degree is not more than the above upper limit, the moisture resistance of the interlayer film and the laminated glass is increased.

  The degree of acetylation is a value indicating the mole fraction obtained by dividing the amount of ethylene groups to which acetyl groups are bonded by the total amount of ethylene groups in the main chain, as a percentage. The amount of ethylene group to which the acetyl group is bonded can be measured, for example, according to JIS K6728 “Testing method for polyvinyl butyral”.

  The degree of acetalization (degree of butyralization in the case of polyvinyl butyral resin) of the polyvinyl acetal resin (2) and the polyvinyl acetal resin (3) is preferably 55 mol% or more, more preferably 60 mol% or more, preferably Is 75 mol% or less, more preferably 71 mol% or less. When the degree of acetalization is not less than the above lower limit, the compatibility between the polyvinyl acetal resin and the plasticizer increases. When the degree of acetalization is less than or equal to the above upper limit, the reaction time required for producing a polyvinyl acetal resin is shortened.

  The degree of acetalization is the value obtained by subtracting the amount of ethylene groups bonded with hydroxyl groups and the amount of ethylene groups bonded with acetyl groups from the total amount of ethylene groups of the main chain. It is a value indicating the mole fraction obtained by dividing by the percentage.

  The hydroxyl group content (hydroxyl group amount), acetalization degree (butyralization degree), and acetylation degree are preferably calculated from results measured by a method based on JIS K6728 “Testing methods for polyvinyl butyral”. However, you may use the measurement by ASTM D1396-92. When the polyvinyl acetal resin is a polyvinyl butyral resin, the hydroxyl group content (hydroxyl content), the acetalization degree (butyralization degree), and the acetylation degree are determined in accordance with JIS K6728 “Testing methods for polyvinyl butyral”. It can be calculated from the results measured by

(Plasticizer)
From the viewpoint of effectively improving sound insulation, the first layer includes a plasticizer (hereinafter sometimes referred to as a plasticizer (1)). The plasticizer (1) is selected in consideration of the first configuration and the second configuration. As for the said plasticizer (1), only 1 type may be used and 2 or more types may be used together.

  From the viewpoint of effectively improving sound insulation, the second layer includes a plasticizer (hereinafter, may be referred to as a plasticizer (2)). From the viewpoint of effectively improving sound insulation, the third layer preferably contains a plasticizer (hereinafter, sometimes referred to as a plasticizer (3)). As for the plasticizer in these layers, only 1 type may be used and 2 or more types may be used together.

  Examples of the plasticizer include paraffin oil, organic ester plasticizer, and organic phosphate plasticizer. Examples of the organic ester plasticizer include monobasic organic acid esters and polybasic organic acid esters. Examples of the phosphoric acid plasticizer include organic phosphoric acid plasticizers and organic phosphorous acid plasticizers. The plasticizer is preferably a liquid plasticizer.

  Examples of the paraffin oil include naphthenic process oil, white mineral oil, mineral oil, paraffin wax, and liquid paraffin.

  Examples of the commercially available paraffin oil include “Diana Process Oil PW-90” manufactured by Idemitsu Kosan Co., Ltd., “Diana Process Oil PW-100” manufactured by Idemitsu Kosan Co., Ltd., and “Diana Process Oil PW-32” manufactured by Idemitsu Kosan Co., Ltd. It is done.

  Examples of the organic ester plasticizer include triethylene glycol di-2-ethylpropanoate, triethylene glycol di-2-ethylbutyrate, triethylene glycol di-2-ethylhexanoate, triethylene glycol dicaprylate, Triethylene glycol di-n-octanoate, triethylene glycol di-n-heptanoate, tetraethylene glycol di-n-heptanoate, dibutyl sebacate, dioctyl azelate, dibutyl carbitol adipate, ethylene glycol di-2-ethylbutyrate, 1,3-propylene glycol di-2-ethyl butyrate, 1,4-butylene glycol di-2-ethyl butyrate, diethylene glycol di-2-ethyl butyrate, diethylene glycol di-2-ethyl Xanoate, dipropylene glycol di-2-ethylbutyrate, triethylene glycol di-2-ethylpentanoate, tetraethylene glycol di-2-ethylbutyrate, diethylene glycol dicaprylate, dihexyl adipate, dioctyl adipate, adipine Hexyl cyclohexyl, a mixture of heptyl adipate and nonyl adipate, diisononyl adipate, diisodecyl adipate, heptylnonyl adipate, dibutyl sebacate, alkyd oil-modified sebacate, and a mixture of phosphate ester and adipate Can be mentioned. Organic ester plasticizers other than these may be used. Other adipic acid esters other than the above-mentioned adipic acid esters may be used.

  When represented by the structural formula, examples of the organic ester plasticizer include diester plasticizers represented by the following formula (11).

  In the above formula (11), R1 and R2 each represent an organic group having 5 to 10 carbon atoms, R3 represents an ethylene group, an isopropylene group or an n-propylene group, and p represents an integer of 3 to 10. . R1 and R2 in the above formula (11) are each preferably an organic group having 6 to 10 carbon atoms.

  Examples of the organic phosphate plasticizer include tributoxyethyl phosphate, isodecylphenyl phosphate, triisopropyl phosphate, and the like.

  When the thermoplastic resin of the first layer is a thermoplastic elastomer, the plasticizing effect may be low. When a thermoplastic elastomer is used as the thermoplastic resin of the first layer, the plasticizer in the first layer is preferably a plasticizer other than the organic ester plasticizer.

  From the viewpoint of effectively improving sound insulation, the plasticizer in the first layer is preferably paraffin oil.

  From the viewpoint of effectively increasing the adhesion between the glass and the interlayer film, the plasticizer in the second layer and the plasticizer in the third layer are each preferably an organic ester plasticizer. More preferably, it is a diester plasticizer represented by the above formula (11). From the viewpoint of effectively increasing the adhesion between the glass and the interlayer film, the plasticizer in the second layer and the plasticizer in the third layer are each triethylene glycol di-2-ethylhexa. Preferably, it includes noate (3GO) or triethylene glycol di-2-ethylbutyrate (3GH), and more preferably includes triethylene glycol di-2-ethylhexanoate.

  From the viewpoint of effectively enhancing sound insulation, in the first layer, the content of the plasticizer (1) relative to 100 parts by weight of the thermoplastic resin (1) (hereinafter referred to as content (1)). Is preferably 10 parts by weight or more, more preferably 20 parts by weight or more, preferably 60 parts by weight or less, more preferably 50 parts by weight or less. Moreover, sound insulation can be effectively improved as the said content (1) is more than the said minimum. When the content (1) is not more than the above upper limit, the penetration resistance of the laminated glass is further enhanced.

  The content of the plasticizer (2) with respect to 100 parts by weight of the thermoplastic resin (2) is defined as content (2). The content of the plasticizer (3) with respect to 100 parts by weight of the thermoplastic resin (3) is defined as content (3). The content (2) and the content (3) are each preferably 10 parts by weight or more, more preferably 15 parts by weight or more, still more preferably 20 parts by weight or more, particularly preferably 24 parts by weight or more, and most preferably 25 parts by weight or more, preferably 45 parts by weight or less, more preferably 40 parts by weight or less. When the content (2) and the content (3) are equal to or higher than the lower limit, the flexibility of the intermediate film is increased and the handling of the intermediate film is facilitated. When the content (2) and the content (3) are not more than the upper limit, the penetration resistance of the laminated glass is further enhanced.

(Thermal barrier compound)
The intermediate film preferably contains a heat shielding compound. The first layer preferably contains a heat shielding compound. The second layer preferably contains a heat shielding compound. The third layer preferably includes a heat shielding compound. As for the said heat-shielding compound, only 1 type may be used and 2 or more types may be used together.

  The heat-shielding compound preferably contains at least one component X among phthalocyanine compounds, naphthalocyanine compounds and anthracocyanine compounds, or preferably contains heat-shielding particles. In this case, both the component X and the heat shielding particles may be included.

Component X:
The intermediate film preferably includes at least one component X among a phthalocyanine compound, a naphthalocyanine compound, and an anthracocyanine compound. The first layer preferably contains the component X. The second layer preferably contains the component X. The third layer preferably contains the component X. The component X is a heat shielding compound. As for the said component X, only 1 type may be used and 2 or more types may be used together.

  The component X is not particularly limited. As component X, conventionally known phthalocyanine compounds, naphthalocyanine compounds and anthracocyanine compounds can be used.

  Examples of the component X include phthalocyanine, a derivative of phthalocyanine, naphthalocyanine, a derivative of naphthalocyanine, anthracyanine, an anthracocyanine derivative, and the like. The phthalocyanine compound and the phthalocyanine derivative preferably each have a phthalocyanine skeleton. The naphthalocyanine compound and the naphthalocyanine derivative preferably each have a naphthalocyanine skeleton. It is preferable that each of the anthocyanin compound and the derivative of the anthracyanine has an anthracyanine skeleton.

  From the viewpoint of further increasing the heat shielding properties of the interlayer film and the laminated glass, the component X is preferably at least one selected from the group consisting of phthalocyanine, phthalocyanine derivatives, naphthalocyanine, and naphthalocyanine derivatives. More preferably, it is at least one of phthalocyanine and phthalocyanine derivatives.

  From the viewpoint of effectively increasing the heat shielding property and maintaining the visible light transmittance at a higher level over a long period of time, the component X preferably contains a vanadium atom or a copper atom. The component X preferably contains a vanadium atom, and preferably contains a copper atom. The component X is more preferably at least one of a phthalocyanine containing a vanadium atom or a copper atom and a phthalocyanine derivative containing a vanadium atom or a copper atom. From the viewpoint of further increasing the heat shielding properties of the interlayer film and the laminated glass, the component X preferably has a structural unit in which an oxygen atom is bonded to a vanadium atom.

  In 100% by weight of the intermediate film or 100% by weight of the layer containing the component X (first layer, second layer or third layer), the content of the component X is preferably 0.001% by weight. Above, more preferably 0.005% by weight or more, still more preferably 0.01% by weight or more, particularly preferably 0.02% by weight or more. The content of the component X is preferably 0.2% by weight in 100% by weight of the intermediate film or 100% by weight of the layer containing the component X (first layer, second layer, or third layer). Below, more preferably 0.1% by weight or less, still more preferably 0.05% by weight or less, and particularly preferably 0.04% by weight or less. When the content of the component X is not less than the above lower limit and not more than the above upper limit, the heat shielding property is sufficiently high and the visible light transmittance is sufficiently high. For example, the visible light transmittance can be 70% or more.

Thermal barrier particles:
The intermediate film preferably contains heat shielding particles. The first layer preferably contains the heat shielding particles. The second layer preferably includes the heat shielding particles. The third layer preferably contains the heat shielding particles. The heat shielding particles are heat shielding compounds. By using heat shielding particles, infrared rays (heat rays) can be effectively blocked. As for the said heat-shielding particle, only 1 type may be used and 2 or more types may be used together.

  From the viewpoint of further improving the heat shielding property of the laminated glass, the heat shielding particles are more preferably metal oxide particles. The heat shielding particles are preferably particles (metal oxide particles) formed of a metal oxide.

  Infrared rays having a wavelength longer than 780 nm longer than visible light have a smaller amount of energy than ultraviolet rays. However, infrared rays have a large thermal effect, and when infrared rays are absorbed by a substance, they are released as heat. For this reason, infrared rays are generally called heat rays. By using the heat shielding particles, infrared rays (heat rays) can be effectively blocked. The heat shielding particles mean particles that can absorb infrared rays.

Specific examples of the heat shielding particles include aluminum-doped tin oxide particles, indium-doped tin oxide particles, antimony-doped tin oxide particles (ATO particles), gallium-doped zinc oxide particles (GZO particles), and indium-doped zinc oxide particles (IZO particles). ), Aluminum doped zinc oxide particles (AZO particles), niobium doped titanium oxide particles, sodium doped tungsten oxide particles, cesium doped tungsten oxide particles, thallium doped tungsten oxide particles, rubidium doped tungsten oxide particles, tin doped indium oxide particles (ITO particles) And metal oxide particles such as tin-doped zinc oxide particles and silicon-doped zinc oxide particles, and lanthanum hexaboride (LaB ₆ ) particles. Heat shielding particles other than these may be used. Metal oxide particles are preferred because of their high heat ray shielding function, ATO particles, GZO particles, IZO particles, ITO particles or tungsten oxide particles are more preferred, and ITO particles or tungsten oxide particles are particularly preferred. In particular, tin-doped indium oxide particles (ITO particles) are preferable, and tungsten oxide particles are also preferable because they have a high heat ray shielding function and are easily available.

  From the viewpoint of further increasing the heat shielding properties of the interlayer film and the laminated glass, the tungsten oxide particles are preferably metal-doped tungsten oxide particles. The “tungsten oxide particles” include metal-doped tungsten oxide particles. Specific examples of the metal-doped tungsten oxide particles include sodium-doped tungsten oxide particles, cesium-doped tungsten oxide particles, thallium-doped tungsten oxide particles, and rubidium-doped tungsten oxide particles.

From the viewpoint of further increasing the heat shielding properties of the interlayer film and the laminated glass, cesium-doped tungsten oxide particles are particularly preferable. From the viewpoint of further increasing the heat shielding properties of the interlayer film and the laminated glass, the cesium-doped tungsten oxide particles are preferably tungsten oxide particles represented by the formula: Cs _0.33 WO ₃ .

  The average particle diameter of the heat shielding particles is preferably 0.01 μm or more, more preferably 0.02 μm or more, preferably 0.1 μm or less, more preferably 0.05 μm or less. When the average particle size is not less than the above lower limit, the heat ray shielding property is sufficiently increased. When the average particle size is not more than the above upper limit, the dispersibility of the heat shielding particles is increased.

  The “average particle diameter” indicates a volume average particle diameter. The average particle diameter can be measured using a particle size distribution measuring apparatus (“UPA-EX150” manufactured by Nikkiso Co., Ltd.) or the like.

  The content of the heat-shielding particles is preferably 0.01 in 100% by weight of the intermediate film or 100% by weight of the layer containing the heat-shielding particles (first layer, second layer, or third layer). % By weight or more, more preferably 0.1% by weight or more, further preferably 1% by weight or more, and particularly preferably 1.5% by weight or more. The content of the heat shielding particles is preferably 6% by weight in 100% by weight of the intermediate film or 100% by weight of the layer containing the heat shielding particles (first layer, second layer or third layer). Hereinafter, it is more preferably 5.5% by weight or less, further preferably 4% by weight or less, particularly preferably 3.5% by weight or less, and most preferably 3% by weight or less. When the content of the heat shielding particles is not less than the above lower limit and not more than the above upper limit, the heat shielding property is sufficiently high and the visible light transmittance is sufficiently high.

(Metal salt)
The interlayer film preferably contains an alkali metal salt, an alkaline earth metal salt, or a magnesium salt (hereinafter sometimes referred to as a metal salt M). The first layer preferably includes the metal salt M. The second layer preferably contains the metal salt M. The third layer preferably contains the metal salt M. Use of the metal salt M makes it easy to control the adhesion between the interlayer film and a laminated glass member such as a glass plate or the adhesion between the layers in the interlayer film. As for the said metal salt M, only 1 type may be used and 2 or more types may be used together.

  The metal salt M preferably contains Li, Na, K, Rb, Cs, Mg, Ca, Sr or Ba as a metal. The metal salt contained in the intermediate film preferably contains a K salt or an Mg salt.

  The metal salt M is an alkali metal salt of an organic acid having 2 to 16 carbon atoms, an alkaline earth metal salt of an organic acid having 2 to 16 carbon atoms, or a magnesium salt of an organic acid having 2 to 16 carbon atoms. Is more preferable, and it is still more preferable that they are a C2-C16 carboxylic acid magnesium salt or a C2-C16 carboxylic acid potassium salt.

  The said C2-C16 carboxylic acid magnesium salt and the said C2-C16 carboxylic acid potassium salt are not specifically limited. Examples of these include magnesium acetate, potassium acetate, magnesium propionate, potassium propionate, magnesium 2-ethylbutyrate, potassium 2-ethylbutanoate, magnesium 2-ethylhexanoate, and potassium 2-ethylhexanoate. It is done.

  The total content of Mg and K in the intermediate film containing the metal salt M or the layer containing the metal salt M (the first layer, the second layer, or the third layer) is preferably 5 ppm or more. Preferably it is 10 ppm or more, More preferably, it is 20 ppm or more. The total content of Mg and K in the intermediate film containing the metal salt M or the layer containing the metal salt M (the first layer, the second layer, or the third layer) is preferably 300 ppm or less. Preferably it is 250 ppm or less, More preferably, it is 200 ppm or less. When the total content of Mg and K is not less than the above lower limit and not more than the above upper limit, the adhesion between the interlayer film and the glass plate or the adhesion between the layers in the interlayer film can be controlled even better.

(UV shielding agent)
The intermediate film preferably contains an ultraviolet shielding agent. The first layer preferably contains an ultraviolet shielding agent. The second layer preferably contains an ultraviolet shielding agent. The third layer preferably contains an ultraviolet shielding agent. By using the ultraviolet shielding agent, even if the interlayer film and the laminated glass are used for a long period of time, the visible light transmittance is more unlikely to decrease. As for the said ultraviolet shielding agent, only 1 type may be used and 2 or more types may be used together.

  The ultraviolet shielding agent includes an ultraviolet absorber. The ultraviolet shielding agent is preferably an ultraviolet absorber.

  Examples of the ultraviolet shielding agent include an ultraviolet shielding agent containing a metal atom, an ultraviolet shielding agent containing a metal oxide, an ultraviolet shielding agent having a benzotriazole structure (benzotriazole compound), and an ultraviolet shielding agent having a benzophenone structure (benzophenone compound). ), UV screening agent having triazine structure (triazine compound), UV screening agent having malonate ester structure (malonic acid ester compound), UV screening agent having oxalic acid anilide structure (oxalic acid anilide compound) and benzoate structure Examples thereof include an ultraviolet shielding agent (benzoate compound).

  Examples of the ultraviolet shielding agent containing a metal atom include platinum particles, particles in which the surface of the platinum particles is coated with silica, palladium particles, particles in which the surface of the palladium particles is coated with silica, and the like. The ultraviolet shielding agent is preferably not a heat shielding particle.

  The ultraviolet shielding agent is preferably an ultraviolet shielding agent having a benzotriazole structure, an ultraviolet shielding agent having a benzophenone structure, an ultraviolet shielding agent having a triazine structure, or an ultraviolet shielding agent having a benzoate structure. The ultraviolet shielding agent is more preferably an ultraviolet shielding agent having a benzotriazole structure or an ultraviolet shielding agent having a benzophenone structure, and more preferably an ultraviolet shielding agent having a benzotriazole structure.

  Examples of the ultraviolet shielding agent containing the metal oxide include zinc oxide, titanium oxide, and cerium oxide. Furthermore, the surface may be coat | covered regarding the ultraviolet-ray shielding agent containing the said metal oxide. Examples of the coating material on the surface of the ultraviolet shielding agent containing the metal oxide include insulating metal oxides, hydrolyzable organosilicon compounds, and silicone compounds.

  Examples of the insulating metal oxide include silica, alumina and zirconia. The insulating metal oxide has a band gap energy of 5.0 eV or more, for example.

  Examples of the ultraviolet shielding agent having the benzotriazole structure include 2- (2′-hydroxy-5′-methylphenyl) benzotriazole (“TinvinP” manufactured by BASF), 2- (2′-hydroxy-3 ′, 5′-di-t-butylphenyl) benzotriazole (“Tinvin 320” manufactured by BASF), 2- (2′-hydroxy-3′-t-butyl-5-methylphenyl) -5-chlorobenzotriazole (BASF) “Tinuvin 326”), 2- (2′-hydroxy-3 ′, 5′-di-amylphenyl) benzotriazole (“Tinvin 328” manufactured by BASF), and the like. Since the performance of shielding ultraviolet rays is excellent, the ultraviolet shielding agent is preferably an ultraviolet shielding agent having a benzotriazole structure containing a halogen atom, and may be an ultraviolet shielding agent having a benzotriazole structure containing a chlorine atom. More preferred.

  Examples of the ultraviolet shielding agent having the benzophenone structure include octabenzone (“Chimasorb 81” manufactured by BASF).

  Examples of the ultraviolet shielding agent having the triazine structure include “LA-F70” manufactured by ADEKA and 2- (4,6-diphenyl-1,3,5-triazin-2-yl) -5-[(hexyl). And oxy] -phenol ("Tinuvin 1577FF" manufactured by BASF).

  Examples of the ultraviolet screening agent having a malonic ester structure include dimethyl 2- (p-methoxybenzylidene) malonate, tetraethyl-2,2- (1,4-phenylenedimethylidene) bismalonate, and 2- (p-methoxybenzylidene). -Bis (1,2,2,6,6-pentamethyl 4-piperidinyl) malonate and the like.

  Examples of commercially available ultraviolet screening agents having the malonic ester structure include Hostavin B-CAP, Hostavin PR-25, and Hostavin PR-31 (all manufactured by Clariant).

  Examples of the ultraviolet shielding agent having the oxalic anilide structure include N- (2-ethylphenyl) -N ′-(2-ethoxy-5-t-butylphenyl) oxalic acid diamide, N- (2-ethylphenyl)- Oxalic acid diamide having an aryl group substituted on the nitrogen atom, such as N ′-(2-ethoxy-phenyl) oxalic acid diamide, 2-ethyl-2′-ethoxy-oxyanilide (“Slandor VSU” manufactured by Clariant) Kind.

  Examples of the ultraviolet shielding agent having the benzoate structure include 2,4-di-tert-butylphenyl-3,5-di-tert-butyl-4-hydroxybenzoate (“Tinuvin 120” manufactured by BASF). .

  In 100% by weight of the layer containing the ultraviolet screening agent (first layer, second layer or third layer), the content of the ultraviolet screening agent is preferably 0.1% by weight or more, more preferably 0%. .2% by weight or more, more preferably 0.3% by weight or more, and particularly preferably 0.5% by weight or more. In 100% by weight of the layer containing the ultraviolet shielding agent (first layer, second layer or third layer), the content of the ultraviolet shielding agent is preferably 2.5% by weight or less, more preferably 2%. % By weight or less, more preferably 1% by weight or less, particularly preferably 0.8% by weight or less. When the content of the ultraviolet shielding agent is not less than the above lower limit and not more than the above upper limit, a decrease in visible light transmittance after a lapse of time is further suppressed. In particular, in 100% by weight of the layer containing the ultraviolet shielding agent, the visible light transmittance after a period of the resin film and the glass plate-containing laminate is obtained because the content of the ultraviolet shielding agent is 0.2% by weight or more. Can be remarkably suppressed.

(Antioxidant)
The intermediate film preferably contains an antioxidant. The first layer preferably contains an antioxidant. The second layer preferably contains an antioxidant. The third layer preferably contains an antioxidant. As for the said antioxidant, only 1 type may be used and 2 or more types may be used together.

  Examples of the antioxidant include phenol-based antioxidants, sulfur-based antioxidants, and phosphorus-based antioxidants. The phenolic antioxidant is an antioxidant having a phenol skeleton. The sulfur-based antioxidant is an antioxidant containing a sulfur atom. The phosphorus antioxidant is an antioxidant containing a phosphorus atom.

  The antioxidant is preferably a phenolic antioxidant or a phosphorus antioxidant.

  Examples of the phenolic antioxidant include 2,6-di-t-butyl-p-cresol (BHT), butylhydroxyanisole (BHA), 2,6-di-t-butyl-4-ethylphenol, stearyl- β- (3,5-di-t-butyl-4-hydroxyphenyl) propionate, 2,2′-methylenebis- (4-methyl-6-butylphenol), 2,2′-methylenebis- (4-ethyl-6) -T-butylphenol), 4,4'-butylidene-bis- (3-methyl-6-t-butylphenol), 1,1,3-tris- (2-methyl-hydroxy-5-t-butylphenyl) butane Tetrakis [methylene-3- (3 ′, 5′-butyl-4-hydroxyphenyl) propionate] methane, 1,3,3-tris- (2-methyl-4-hydride) Xyl-5-tert-butylphenol) butane, 1,3,5-trimethyl-2,4,6-tris (3,5-di-tert-butyl-4-hydroxybenzyl) benzene, bis (3,3′- and t-butylphenol) butyric acid glycol ester and bis (3-t-butyl-4-hydroxy-5-methylbenzenepropanoic acid) ethylene bis (oxyethylene). One or more of these antioxidants are preferably used.

  Examples of the phosphorus antioxidant include tridecyl phosphite, tris (tridecyl) phosphite, triphenyl phosphite, trinonylphenyl phosphite, bis (tridecyl) pentaerythritol diphosphite, bis (decyl) pentaerythritol diphos. Phyto, tris (2,4-di-t-butylphenyl) phosphite, bis (2,4-di-t-butyl-6-methylphenyl) ethyl ester phosphorous acid, and 2,2′-methylenebis (4 , 6-di-t-butyl-1-phenyloxy) (2-ethylhexyloxy) phosphorus and the like. One or more of these antioxidants are preferably used.

  Examples of commercially available antioxidants include “IRGANOX 245” manufactured by BASF, “IRGAFOS 168” manufactured by BASF, “IRGAFOS 38” manufactured by BASF, “Smilizer BHT” manufactured by Sumitomo Chemical Co., Ltd., and Sakai Chemical Industry “H-BHT”, “IRGANOX 1010” manufactured by BASF, and the like can be mentioned.

  In order to maintain the high visible light transmittance of the interlayer film and the laminated glass over a long period of time, a layer (first layer, second layer or third layer) in 100% by weight of the interlayer film or containing an antioxidant. ) In 100% by weight, the content of the antioxidant is preferably 0.1% by weight or more. Further, since the effect of adding the antioxidant is saturated, the content of the antioxidant is preferably 2% by weight or less in 100% by weight of the intermediate film or 100% by weight of the layer containing the antioxidant. .

(Other ingredients)
Each of the intermediate film, the first layer, the second layer, and the third layer may contain other components as necessary. The other components include a coupling agent, a dispersant, a surfactant, a flame retardant, an antistatic agent, a pigment, a dye, an adhesive strength regulator (metal salt) between the laminated glass member and the layer in contact with the laminated glass member. Excluded), interlayer adhesion adjusting agent (excluding metal salts), moisture-proofing agent, fluorescent brightening agent, infrared absorber and the like. As for said other component, only 1 type may be used and 2 or more types may be used together.

(Other details of interlayer film for laminated glass)
The thickness of the intermediate film is not particularly limited. From the viewpoint of practical use and from the viewpoint of sufficiently enhancing the penetration resistance and bending rigidity of the laminated glass, the thickness of the interlayer film is preferably 0.1 mm or more, more preferably 0.25 mm or more, preferably 3 mm or less, more Preferably it is 1.5 mm or less. When the thickness of the interlayer film is not less than the above lower limit, the penetration resistance and bending rigidity of the laminated glass are further increased. When the thickness of the interlayer film is not more than the above upper limit, the transparency of the interlayer film is further improved.

  Let T be the thickness of the intermediate film. The thickness of the first layer is preferably 0.035T or more, more preferably 0.0625T or more, further preferably 0.1T or more, preferably 0.4T or less, more preferably 0.375T or less, and still more preferably. It is 0.25 T or less, particularly preferably 0.15 T or less. When the thickness of the first layer is 0.4 T or less, the bending rigidity is further improved.

Each thickness of the second layer and the third layer is preferably 0.3 T or more, more preferably 0.3125 T or more, still more preferably 0.375 T or more, preferably 0.97 T or less, more preferably 0. 9375T or less, more preferably 0.9T or less. Each thickness of the second layer and the third layer may be 0.46875T or less, or 0.45T or less. Further, when the thicknesses of the second layer and the third layer are not less than the lower limit and not more than the upper limit, the rigidity and sound insulation of the laminated glass are further enhanced.

  The total thickness of the second layer and the third layer is preferably 0.625 T or more, more preferably 0.75 T or more, still more preferably 0.85 T or more, preferably 0.97 T or less, more preferably 0.9375T or less, more preferably 0.9T or less. Further, when the total thickness of the second layer and the third layer is not less than the above lower limit and not more than the above upper limit, the rigidity and sound insulation of the laminated glass are further enhanced.

  The intermediate film may be an intermediate film having a uniform thickness or an intermediate film having a changed thickness. The cross-sectional shape of the intermediate film may be rectangular or wedge-shaped. The intermediate film may be wound, and the intermediate film may be a roll body.

  The method for producing the interlayer film according to the present invention is not particularly limited. Examples of the method for producing an interlayer film according to the present invention include a method of extruding a resin composition using an extruder in the case of a single-layer interlayer film. As a method for producing an intermediate film according to the present invention, in the case of a multilayer intermediate film, for example, a method of laminating each obtained layer after forming each layer using each resin composition for forming each layer In addition, a method of laminating each layer by coextruding each resin composition for forming each layer using an extruder may be used. Further, from the viewpoint of effectively improving the adhesion between the interlayers of the intermediate film, a method of laminating after the plasma treatment or the corona treatment on the first layer is also mentioned. Since it is suitable for continuous production, an extrusion method is preferred.

  It is preferable that the same polyvinyl acetal resin is contained in the second layer and the third layer, and the same polyvinyl acetal resin and the same are contained in the second layer and the third layer. It is more preferable that a plasticizer is included, and it is more preferable that the second layer and the third layer are formed of the same resin composition. In this case, the production efficiency of the intermediate film is excellent.

  The intermediate film preferably has an uneven shape on at least one of the surfaces on both sides. More preferably, the intermediate film has a concavo-convex shape on both surfaces. It does not specifically limit as a method of forming said uneven | corrugated shape, For example, a lip embossing method, an embossing roll method, a calendering roll method, a profile extrusion method, etc. are mentioned. The embossing roll method is preferable because it can form a large number of concavo-convex embossments that are quantitatively constant.

(Laminated glass)
FIG. 2 is a cross-sectional view schematically showing an example of a laminated glass using the laminated glass interlayer film shown in FIG.

  A laminated glass 31 shown in FIG. 2 includes a first laminated glass member 21, a second laminated glass member 22, and the intermediate film 11. The intermediate film 11 is disposed between the first laminated glass member 21 and the second laminated glass member 22 and is sandwiched.

  A first laminated glass member 21 is laminated on the first surface 11 a of the intermediate film 11. A second laminated glass member 22 is laminated on the second surface 11 b opposite to the first surface 11 a of the intermediate film 11. A first laminated glass member 21 is laminated on the outer surface 2 a of the second layer 2. A second laminated glass member 22 is laminated on the outer surface 3 a of the third layer 3.

  Thus, the laminated glass which concerns on this invention is equipped with the 1st laminated glass member, the 2nd laminated glass member, and the intermediate film, and this intermediate film is the intermediate film for laminated glasses which concerns on this invention. It is. In the laminated glass according to the present invention, the interlayer film is disposed between the first laminated glass member and the second laminated glass member.

  The first laminated glass member is preferably a first glass plate. The second laminated glass member is preferably a second glass plate.

  Examples of the laminated glass member include a glass plate and a PET (polyethylene terephthalate) film. Laminated glass includes not only laminated glass in which an intermediate film is sandwiched between two glass plates, but also laminated glass in which an intermediate film is sandwiched between a glass plate and a PET film or the like. The laminated glass is a laminate including a glass plate, and preferably at least one glass plate is used. Each of the first laminated glass member and the second laminated glass member is a glass plate or a PET film, and the laminated glass is one of the first laminated glass member and the second laminated glass member. It is preferable to provide a glass plate as at least one.

  Examples of the glass plate include inorganic glass and organic glass. Examples of the inorganic glass include float plate glass, heat ray absorbing plate glass, heat ray reflecting plate glass, polished plate glass, mold plate glass, and wire-containing plate glass. The organic glass is a synthetic resin glass substituted for inorganic glass. Examples of the organic glass include polycarbonate plates and poly (meth) acrylic resin plates. Examples of the poly (meth) acrylic resin plate include a polymethyl (meth) acrylate plate.

  The thickness of the laminated glass member is preferably 1 mm or more, more preferably 1.8 mm or more, further preferably 2 mm or more, particularly preferably 2.1 mm or more, preferably 5 mm or less, more preferably 3 mm or less. Further, when the laminated glass member is a glass plate, the thickness of the glass plate is preferably 1 mm or more, more preferably 1.8 mm or more, further preferably 2 mm or more, particularly preferably 2.1 mm or more, preferably It is 5 mm or less, More preferably, it is 3 mm or less, More preferably, it is 2.6 mm or less. When the laminated glass member is a PET film, the thickness of the PET film is preferably 0.03 mm or more, and preferably 0.5 mm or less.

  The manufacturing method of the said laminated glass is not specifically limited. For example, the intermediate film is sandwiched between the first laminated glass member and the second laminated glass member, passed through a pressing roll, or put in a rubber bag and sucked under reduced pressure, and the first The air remaining between the laminated glass member, the second laminated glass member and the intermediate film is degassed. Then, it pre-adheres at about 70-110 degreeC, and a laminated body is obtained. Next, the laminated body is put in an autoclave or pressed, and pressed at about 120 to 150 ° C. and a pressure of 1 to 1.5 MPa. In this way, a laminated glass can be obtained. You may laminate | stack a 1st layer, a 2nd layer, and a 3rd layer at the time of manufacture of the said laminated glass.

  The interlayer film and the laminated glass can be used for automobiles, railway vehicles, aircraft, ships, buildings, and the like. The said intermediate film and the said laminated glass can be used besides these uses. The interlayer film and the laminated glass are preferably a vehicle or architectural interlayer film and a laminated glass, and more preferably a vehicle interlayer film and a laminated glass. The intermediate film and the laminated glass can be used for an automobile windshield, side glass, rear glass, roof glass, or the like. The interlayer film and the laminated glass are suitably used for automobiles. The interlayer film is used for obtaining laminated glass for automobiles.

  Hereinafter, the present invention will be described in more detail with reference to examples and comparative examples. The present invention is not limited to these examples.

Example 1
Preparation of interlayer film:
Aliphatic polyolefin (“Absotemer EP-1001” manufactured by Mitsui Chemicals, Inc .; thermoplastic elastomer) was dissolved at 25% by weight with respect to toluene to obtain a toluene solution. To the toluene solution, 35 parts by weight of paraffin oil paraffin oil (“Diana Process Oil PW-32” manufactured by Idemitsu Kosan Co., Ltd.) was added to 100 parts by weight of Abssorter, and stirred uniformly. Next, this solution was apply | coated on the PET film which carried out the mold release process so that the thickness after drying might be set to 50 micrometers using a coater, and it was made to dry at 120 degreeC for 1 hour, and the resin film was obtained. The obtained resin film having a thickness of 50 μm was overlapped to obtain a first layer having a thickness of 100 μm.

  Further, one surface of the first layer was irradiated with plasma, and immediately after that, a second layer having a thickness of 350 μm was bonded to the plasma irradiation surface.

Formulation composition of the second layer:
Polyvinyl acetal resin (average polymerization degree 1700, using n-butyraldehyde, acetalization degree 68.5 mol%, hydroxyl group content 30.7 mol%, acetylation degree 0.8 mol%) 100 parts by weight Triethylene glycol 35 parts by weight of di-2-ethylhexanoate (3GO) In an intermediate film from which an ultraviolet screening agent (2- (2-hydroxy-3-tert-butyl-5-methylphenyl) -5-chlorobenzotriazole) can be obtained An amount of 0.2% by weight An amount of 0.2% by weight in an intermediate film from which an antioxidant (2,6-di-t-butyl-p-cresol) can be obtained

  Next, the other surface of the first layer was irradiated with plasma in the same manner, and a third layer having a thickness of 350 μm (the same composition as the second layer) was bonded.

  An intermediate film (thickness 800 μm) having a laminated structure of second layer (thickness 350 μm) / first layer (thickness 100 μm) / third layer (thickness 350 μm) was produced.

Laminated glass production:
The obtained intermediate film was cut into a size of 30 cm long × 2.5 cm wide. As the first laminated glass member and the second laminated glass member, two glass plates (clear float glass, thickness 2 mm, length 30 cm × width 2.5 cm) were prepared. An interlayer film was sandwiched between two glass plates to obtain a laminate. This laminated body is put in a rubber bag, deaerated at a vacuum degree of 2.6 kPa for 20 minutes, transferred to an oven while being deaerated, and further kept at 90 ° C. for 30 minutes and vacuum-pressed. Crimped. The pre-pressed laminate was pressed for 20 minutes in an autoclave at 135 ° C. and a pressure of 1.2 MPa to obtain a laminated glass.

(Example 2)
In the same manner as in Example 1, except that the blending amount of the paraffin oil “Diana Process Oil PW-32”) in the composition for forming the first layer was changed to 40 parts by weight, A film and laminated glass were obtained.

(Comparative Example 1)
Preparation of a composition for forming the first layer:
The following components were blended and sufficiently kneaded with a mixing roll to obtain a composition for forming the first layer.

Polyvinyl acetal resin (average polymerization degree 3050, using n-butyraldehyde, acetalization degree 63.7 mol%, hydroxyl group content 24.2 mol%, acetylation degree 12.1 mol%)
60 parts by weight of triethylene glycol di-2-ethylhexanoate (3GO) Intermediate for obtaining an ultraviolet shielding agent (2- (2-hydroxy-3-tert-butyl-5-methylphenyl) -5-chlorobenzotriazole) An amount of 0.2% by weight in the film An amount of 0.2% by weight in the intermediate film from which the antioxidant (2,6-di-t-butyl-p-cresol) can be obtained

Production of compositions for forming the second and third layers:
The following components were blended and sufficiently kneaded with a mixing roll to obtain a composition for forming the second layer and the third layer.

Polyvinyl acetal resin (average polymerization degree 1700, using n-butyraldehyde, acetalization degree 68.5 mol%, hydroxyl group content 30.7 mol%, acetylation degree 0.8 mol%) 100 parts by weight Triethylene glycol 39.5 parts by weight of di-2-ethylhexanoate (3GO) Intermediate film from which an ultraviolet screening agent (2- (2-hydroxy-3-tert-butyl-5-methylphenyl) -5-chlorobenzotriazole) can be obtained The amount which becomes 0.2% by weight in the amount which becomes 0.2% by weight in the intermediate film from which the antioxidant (2,6-di-t-butyl-p-cresol) can be obtained.

Preparation of interlayer film:
The composition for forming the first layer and the composition for forming the second layer and the third layer are coextruded using a coextrusion machine, whereby the second layer (thickness) An intermediate film (thickness 800 μm) having a laminated structure of 350 μm) / first layer (thickness 100 μm) / third layer (thickness 350 μm) was produced.

  A laminated glass was obtained in the same manner as in Example 1 except that the above-described composition for forming each layer was used and an intermediate film was produced by the above-described method.

(Evaluation)
(1) Temperature at which clouding occurs 1 and liquid no. 2 were prepared.

Liquid No. 1: Liquid No. 1 in which 100 parts by weight of the plasticizer in the first layer was mixed with 8 parts by weight of the thermoplastic resin in the second layer. 2: Liquid obtained by mixing 8 parts by weight of the thermoplastic resin in the first layer with 100 parts by weight of the plasticizer in the second layer.

  In addition, liquid No. 1 is the same as the liquid obtained by mixing 8 parts by weight of the thermoplastic resin in the third layer with 100 parts by weight of the plasticizer in the first layer. Liquid No. 2 is the same as the liquid obtained by mixing 8 parts by weight of the thermoplastic resin in the first layer with 100 parts by weight of the plasticizer in the third layer.

  The liquid No. For 1, the temperature at which clouding occurred was determined according to the first cloud point determination method and the second cloud point determination method described above. The temperature at which fogging occurred was determined according to the following criteria.

[Temperature at which cloudiness occurs]
A: Not completely dissolved at 180 ° C. B: Completely dissolved at 180 ° C. and no clouding occurs at 180 ° C., but clouding occurs at 130 ° C. or higher. C: Completely melts at 180 ° C. and below 130 ° C. Cloudy

  The liquid No. For 2, the temperature at which clouding occurred was determined according to the first cloud point determination method and the second cloud point determination method described above. The temperature at which fogging occurred was determined according to the following criteria.

[Temperature at which cloudiness occurs]
A: Not completely dissolved at 180 ° C. B: Completely dissolved at 180 ° C. and cloudy at 50 ° C. or higher C: Completely melted at 180 ° C. and clouded at less than 50 ° C.

(2) Glass transition temperature and tan δ
The obtained interlayer film was stored for one month in an environment of room temperature 23 ± 2 ° C. and humidity 25 ± 5%. Immediately after storage, the thickness of the first layer obtained by peeling the second layer and the third layer from the intermediate film in an environment of room temperature 23 ± 2 ° C. is 0.35 mm. A resin film was produced by press molding at 150 ° C. (150 ° C. for 10 minutes without pressure, and 150 ° C. for 10 minutes with pressure). Then, about this resin film, viscoelasticity was measured using "ARES-G2" by TA Instruments. As a jig, using a parallel plate with a diameter of 8 mm, the glass transition temperature and tan δ are set under the condition that the temperature is lowered from 100 ° C. to −50 ° C. at a temperature drop rate of 3 ° C./min, and the frequency is 1 Hz and the strain is 1%. It was measured.

(3) Sound insulation stability The obtained interlayer film was cut into a size of 25 mm in width and 300 mm in length. Two glass plates (clear float glass, width 25 mm, length 300 mm, and thickness 2 mm) were prepared as the first laminated glass member and the second laminated glass member. An interlayer film was sandwiched between two glass plates to obtain a laminate. This laminated body is put in a rubber bag, deaerated at a vacuum degree of 2.6 kPa for 20 minutes, transferred to an oven while being deaerated, and further kept at 90 ° C. for 30 minutes and vacuum-pressed. Crimped. The pre-pressed laminate was pressed for 20 minutes in an autoclave at 135 ° C. and a pressure of 1.2 MPa to obtain a laminated glass. The obtained laminated glass was stored in an environment of room temperature 23 ± 2 ° C. and humidity 25 ± 5%.

  The obtained laminated glass was vibrated in a constant temperature bath at 20 ° C. with a vibration generator for a damping test (“Vibrator G21-005D” manufactured by Senken). The vibration characteristics obtained therefrom were amplified by a mechanical impedance measuring device (“XG-81” manufactured by Lion Co., Ltd.), and the vibration spectrum was analyzed by an FFT spectrum analyzer (“FFT analyzer HP3582A” manufactured by Yokogawa Hewlett-Packard Company).

  Let α be the resonance frequency of the secondary mode obtained by vibrating the laminated glass 24 hours after the completion of the autoclave. Further, β represents the resonance frequency of the secondary mode obtained by vibrating the laminated glass 4 weeks after the completion of the autoclave. The smaller the change from α to β, the more stable the sound insulation with time. Using γ = | β−α | as an index indicating the stability of sound insulation, the stability of sound insulation was determined according to the following criteria.

[Sound insulation stability criteria]
○: γ is less than 80 Hz △: γ is 80 Hz or more and less than 100 Hz ×: γ is 100 Hz or more

(4) Sound insulation property The obtained interlayer film was cut into a width of 500 mm and a length of 500 mm. Two glass plates (clear float glass, width 500 mm, length 500 mm, and thickness 2 mm) were prepared as the first laminated glass member and the second laminated glass member. An interlayer film was sandwiched between two glass plates to obtain a laminate. This laminated body is put in a rubber bag, deaerated at a vacuum degree of 2.6 kPa for 20 minutes, transferred to an oven while being deaerated, and further kept at 90 ° C. for 30 minutes and vacuum-pressed. Crimped. The pre-pressed laminate was pressed for 20 minutes in an autoclave at 135 ° C. and a pressure of 1.2 MPa to obtain a laminated glass. The obtained laminated glass was stored for 1 month in an environment of room temperature 23 ± 2 ° C. and humidity 25 ± 5%.

  The sound transmission loss of the obtained laminated glass was measured by a method based on JIS A 1441-1, and the sound insulation was determined from the value of sound transmission loss at 3150 Hz close to the coincidence frequency according to the following criteria.

[Criteria for sound insulation]
○: 40 dB or more Δ: 35 dB or more, less than 40 dB ×: less than 35 dB

  Details and results are shown in Table 1 below.

DESCRIPTION OF SYMBOLS 1 ... 1st layer 1a ... 1st surface 1b ... 2nd surface 2 ... 2nd layer 2a ... Outer surface 3 ... 3rd layer 3a ... Outer surface 11 ... Intermediate film 11a ... 1st surface 11b ... 2nd surface 21 ... 1st laminated glass member 22 ... 2nd laminated glass member 31 ... Laminated glass

Claims (12)

A first layer comprising a thermoplastic resin and a plasticizer;
A second layer comprising a thermoplastic resin and a plasticizer,
The second layer is disposed on the first surface side of the first layer,
The combination of the thermoplastic resin in the second layer and the plasticizer in the first layer is such that the heat in the second layer is added to 100 parts by weight of the plasticizer in the first layer. It is a combination that does not completely dissolve at 180 ° C. in a liquid mixed with 8 parts by weight of a plastic resin, or the thermoplasticity in the second layer is added to 100 parts by weight of the plasticizer in the first layer. An interlayer film for laminated glass, which is a combination in which clouding does not occur at 180 ° C. in a liquid mixed with 8 parts by weight of resin and clouding occurs at 130 ° C. or higher when the temperature of the liquid is lowered from 180 ° C.   The combination of the thermoplastic resin in the first layer and the plasticizer in the second layer is such that the heat in the first layer is added to 100 parts by weight of the plasticizer in the second layer. It is a combination that does not completely dissolve at 180 ° C. in a liquid mixed with 8 parts by weight of a plastic resin, or 100 parts by weight of the plasticizer in the second layer and the thermoplasticity in the first layer. The laminated glass according to claim 1, which is a combination in which clouding does not occur at 180 ° C. in a liquid mixed with 8 parts by weight of resin and clouding occurs at 50 ° C. or more when the temperature of the liquid is lowered from 180 ° C. Interlayer film.   The interlayer film for laminated glass according to claim 1 or 2, wherein the thermoplastic resin in the first layer is a thermoplastic elastomer.   The interlayer film for laminated glass according to claim 3, wherein the thermoplastic elastomer is an aliphatic polyolefin.   The interlayer film for laminated glass according to claim 4, wherein the aliphatic polyolefin is a saturated aliphatic polyolefin.   The interlayer film for laminated glass according to any one of claims 1 to 5, wherein the plasticizer in the first layer is a plasticizer other than an organic ester plasticizer.   The interlayer film for laminated glass according to any one of claims 1 to 6, wherein the plasticizer in the first layer is paraffin oil.   The interlayer film for laminated glass according to any one of claims 1 to 7, wherein the thermoplastic resin in the second layer is a polyvinyl acetal resin. Comprising a third layer comprising a thermoplastic resin and a plasticizer;
The third layer is disposed on a second surface side opposite to the first surface side of the first layer;
The combination of the thermoplastic resin in the third layer and the plasticizer in the first layer is such that the heat in the third layer is added to 100 parts by weight of the plasticizer in the first layer. It is a combination that does not completely dissolve at 180 ° C. in a liquid mixed with 8 parts by weight of a plastic resin, or the thermoplasticity in the third layer is added to 100 parts by weight of the plasticizer in the first layer. 9. A combination in which clouding does not occur at 180 ° C. in a liquid mixed with 8 parts by weight of resin, and clouding occurs at 130 ° C. or higher when the temperature of the liquid is lowered from 180 ° C. 9. The interlayer film for laminated glass according to Item.   The combination of the thermoplastic resin in the first layer and the plasticizer in the third layer is such that the heat in the first layer is added to 100 parts by weight of the plasticizer in the third layer. It is a combination that does not completely dissolve at 180 ° C. in a liquid mixed with 8 parts by weight of a plastic resin, or the thermoplasticity in the first layer is added to 100 parts by weight of the plasticizer in the third layer. The laminated glass according to claim 9, which is a combination in which clouding does not occur at 180 ° C. in a liquid mixed with 8 parts by weight of resin and clouding occurs at 50 ° C. or more when the temperature of the liquid is lowered from 180 ° C. Interlayer film.   The interlayer film for laminated glass according to claim 10, wherein the thermoplastic resin in the third layer is a polyvinyl acetal resin. A first laminated glass member;
A second laminated glass member;
An interlayer film for laminated glass according to any one of claims 1 to 11,
Laminated glass in which the interlayer film for laminated glass is disposed between the first laminated glass member and the second laminated glass member.

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