Intermediate film for laminated glass, and laminated glass

Abstract

The present invention provides an intermediate film for laminated glass capable of suppressing bleed-out and enhancing sound insulation in a medium frequency region.　The intermediate film for laminated glass according to the present invention has a structure consisting of three or more layers, including a first layer, a second layer, and a third layer. The second layer is disposed on a first surface side of the first layer, and the third layer is disposed on a second surface side of the first layer opposite to the first surface. The intermediate film contains a thermoplastic resin and a plasticizer. When the minimum thickness of the first layer is defined as X μm, the content of the plasticizer in the intermediate film per 100 pts.wt. of the thermoplastic resin in the intermediate film is defined as Y pts.wt., and the primary resonance frequency of laminated glass G, obtained by disposing the intermediate film between two clear glass sheets having a thickness of 2.1 mm, is defined as ZHz, the intermediate film has at least one configuration amongst a specific configuration A, a specific configuration B, and a specific configuration C.

Description

Interlayer film for laminated glass and laminated glass

[0001] The present invention relates to an interlayer film for laminated glass used to obtain laminated glass. The present invention also relates to laminated glass using the above interlayer film for laminated glass.

[0002] Laminated glass has an excellent safety performance in that even when damaged by an external impact, the amount of scattered glass fragments is small. Therefore, the above laminated glass is widely used in automobiles, railway vehicles, aircraft, ships, buildings, and the like. The above laminated glass is manufactured by sandwiching an interlayer film for laminated glass between two glass plates.

[0003] As the interlayer film, an interlayer film having a structure of three or more layers is known (for example, Patent Document 1 below).

[0004] Japanese Patent Application Laid-Open No. 2016-108226

[0005] In an interlayer film having a structure of three or more layers, the sound insulation property can be enhanced to a certain extent. However, in a conventional interlayer film having a structure of three or more layers, the sound insulation property in the mid-frequency region (the region of 2500 Hz to 4000 Hz) may not be sufficiently high.

[0006] In order to enhance the sound insulation property in the mid-frequency region, it is conceivable to increase the content of the plasticizer in the intermediate layer of an interlayer film having a structure of three or more layers. However, when the content of the plasticizer in the intermediate layer is simply increased, bleeding out is likely to occur.

[0007] In a conventional interlayer film having a structure of three or more layers, it is difficult to exert both the effects of suppressing bleeding out and enhancing the sound insulation property in the mid-frequency region.

[0008] An object of the present invention is to provide an interlayer film for laminated glass that can suppress bleeding out and enhance the sound insulation property in the mid-frequency region. Another object of the present invention is also to provide laminated glass using the above interlayer film for laminated glass.

[0009] In this specification, the following interlayer film for laminated glass and laminated glass are disclosed.

[0010] Item 1. An interlayer for laminated glass having a structure of three or more layers, comprising a first layer, a second layer, and a third layer, wherein the second layer is disposed on the first surface side of the first layer, and the third layer is disposed on the second surface side of the first layer opposite to the first surface, the interlayer contains a thermoplastic resin and a plasticizer, the minimum thickness of the first layer is X μm, the content of the plasticizer in the interlayer relative to 100 parts by weight of the thermoplastic resin in the interlayer is Y parts by weight, and when the primary resonance frequency of laminated glass G obtained by distributing the interlayer between two clear glass sheets with a thickness of 2.1 mm is Z Hz, the interlayer comprises at least one of the following configurations A, B, and C.

[0011] Configuration A: 125 ≤ X, and 40 ≤ Y ≤ 44

[0012] Configuration B: 125 ≤ X ≤ 250, and -0.0076X + 42.054 ≤ Y ≤ -0.0096X + 45.330

[0013] Configuration C: 125 ≤ X ≤ 250, and 125 ≤ Z ≤ 140

[0014] Item 2. The interlayer is an interlayer for laminated glass according to Item 1, comprising at least the configuration A described above.

[0015] Item 3. The interlayer is an interlayer for laminated glass according to item 1 or 2, comprising at least the configuration B described above.

[0016] Item 4. The interlayer is an interlayer for laminated glass according to any one of items 1 to 3, comprising at least the above-mentioned configuration C.

[0017] Item 5. The interlayer for laminated glass according to any one of items 1 to 4, comprising at least the above-mentioned configuration B and the above-mentioned configuration C.

[0018] Item 6. The interlayer for laminated glass according to any one of items 1 to 5, wherein the first layer comprises a thermoplastic resin and a plasticizer.

[0019] Item 7. The interfilm for laminated glass according to Item 6, wherein the thermoplastic resin in the first layer is a polyvinyl acetal resin.

[0020] Item 8. The interlayer for laminated glass according to any one of items 1 to 7, wherein the second layer comprises a thermoplastic resin and a plasticizer, and the third layer comprises a thermoplastic resin and a plasticizer.

[0021] Item 9. The interlayer film for laminated glass according to Item 8, wherein the content of the plasticizer in the first layer relative to 100 parts by weight of the thermoplastic resin in the first layer is greater than the content of the plasticizer in the second layer relative to 100 parts by weight of the thermoplastic resin in the second 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 is greater than the content of the plasticizer in the third layer relative to 100 parts by weight of the thermoplastic resin in the third layer.

[0022] Item 10. An interlayer for laminated glass according to any one of items 1 to 9, wherein the ratio of the minimum thickness of the first layer to the minimum thickness of the interlayer is 0.14 or more and 0.25 or less.

[0023] Item 11. An interlayer for laminated glass according to any one of items 1 to 10, wherein the glass transition temperature of the first layer is lower than the glass transition temperature of the second layer, and the glass transition temperature of the first layer is lower than the glass transition temperature of the third layer.

[0024] Item 12. Laminated glass comprising a first laminated glass member, a second laminated glass member, and an interlayer for laminated glass according to any one of items 1 to 11, wherein the interlayer is disposed between the first laminated glass member and the second laminated glass member.

[0025] Item 13. Laminated glass comprising a first laminated glass member, a second laminated glass member, and an interlayer for laminated glass having a structure of three or more layers, wherein the interlayer is disposed between the first laminated glass member and the second laminated glass member, the interlayer comprises a first layer, a second layer, and a third layer, the second layer is disposed on the first surface side of the first layer, the third layer is disposed on the second surface side of the first layer opposite to the first surface, the interlayer contains a thermoplastic resin and a plasticizer, the minimum thickness of the first layer is X μm, the content of the plasticizer in the interlayer relative to 100 parts by weight of the thermoplastic resin in the interlayer is Y parts by weight, and the primary resonant frequency of the laminated glass is Z Hz, wherein the laminated glass comprises at least one of the following configurations A, B, and C.

[0026] Configuration A: 125 ≤ X, and 40 ≤ Y ≤ 44

[0027] Configuration B: 125 ≤ X ≤ 250, and -0.0076X + 42.054 ≤ Y ≤ -0.0096X + 45.330

[0028] Configuration C: 125 ≤ X ≤ 250, and 125 ≤ Z ≤ 140

[0029] The interlayer for laminated glass according to the present invention is an interlayer for laminated glass having a structure of three or more layers. The interlayer for laminated glass according to the present invention comprises a first layer, a second layer, and a third layer, wherein the second layer is arranged on the first surface side of the first layer, and the third layer is arranged on the second surface side of the first layer opposite to the first surface. The interlayer for laminated glass according to the present invention contains a thermoplastic resin and a plasticizer. In the present invention, the minimum thickness of the first layer is X μm, the content of the plasticizer in the interlayer relative to 100 parts by weight of the thermoplastic resin in the interlayer is Y parts by weight, and the primary resonance frequency of the laminated glass G obtained by placing the interlayer between two sheets of clear glass with a thickness of 2.1 mm is Z Hz. The interlayer for laminated glass according to the present invention comprises at least one of the specific configurations A, B, and C. The interlayer for laminated glass according to the present invention has the above configuration, which makes it possible to suppress bleed-out and improve sound insulation in the mid-frequency range.

[0030] Figure 1 is a schematic cross-sectional view showing an interlayer for laminated glass according to one embodiment of the present invention. Figure 2 is a schematic cross-sectional view showing an example of laminated glass using the interlayer for laminated glass shown in Figure 1.

[0031] The details of the present invention will be described below.

[0032] (Interlayer for Laminated Glass) The interlayer for laminated glass according to the present invention (hereinafter sometimes abbreviated as "interlayer") has a structure of three or more layers. The interlayer according to the present invention may have a structure of three layers, a structure of three or more layers, a structure of 10 layers or less, or a structure of 5 layers or less.

[0033] The interlayer according to the present invention comprises a first layer, a second layer, and a third layer. The second layer is located on the first surface side of the first layer, and the third layer is located on the second surface side of the first layer, opposite to the first surface.

[0034] The interlayer according to the present invention comprises a thermoplastic resin and a plasticizer.

[0035] In this invention, the minimum thickness of the first layer is set to X μm, the content of the plasticizer in the interlayer relative to 100 parts by weight of the thermoplastic resin in the interlayer is set to Y parts by weight, and the primary resonance frequency of the laminated glass G obtained by placing the interlayer between two clear glass sheets with a thickness of 2.1 mm is set to Z Hz. The unit of X is μm. The unit of Y is parts by weight. The unit of Z is Hz.

[0036] The interlayer according to the present invention comprises at least one of the following configurations A, B, and C.

[0037] Configuration A: 125 ≤ X, and 40 ≤ Y ≤ 44

[0038] Configuration B: 125 ≤ X ≤ 250, and -0.0076X + 42.054 ≤ Y ≤ -0.0096X + 45.330

[0039] Configuration C: 125 ≤ X ≤ 250, and 125 ≤ Z ≤ 140

[0040] The interlayer according to the present invention has the above configuration, which makes it possible to suppress bleed-out and improve sound insulation in the mid-frequency range (2500 Hz to 4000 Hz).

[0041] The interlayer may comprise at least configuration A, at least configuration B, and at least configuration C. The interlayer may comprise at least one configuration from configuration A and configuration B, at least one configuration from configuration A and configuration C, and at least one configuration from configuration B and configuration C. The interlayer may comprise at least configuration A and configuration B, at least configuration A and configuration C, at least configuration B and configuration C, and configuration A, configuration B, and configuration C. The interlayer may comprise at least two configurations from configuration A, configuration B, and configuration C.

[0042] From the perspective of more effectively exerting the effects of the present invention, it is preferable that the intermediate film includes at least the above-described configuration C, and it is more preferable that the intermediate film includes at least the above-described configuration B and the above-described configuration C.

[0043] In the intermediate film including the above-described configuration A, X is 125 or more. That is, in the intermediate film including the above-described configuration A, the minimum thickness of the first layer is 125 μm or more. Further, in the intermediate film including the above-described configuration A, Y is 40 or more and 44 or less. That is, in the intermediate film including the above-described configuration A, the content of the plasticizer in the intermediate film with respect to 100 parts by weight of the thermoplastic resin in the intermediate film is 40 parts by weight or more and 44 parts by weight or less. In the intermediate film including the above-described configuration A, since the minimum thickness of the first layer is relatively thick, the resonance frequency of the laminated glass can be appropriately reduced. Further, in the intermediate film including the above-described configuration A, the content of the plasticizer in the intermediate film is controlled within a specific range. In the intermediate film including the above-described configuration A, the effects of the present invention can be exerted by controlling both the minimum thickness of the first layer and the content of the plasticizer in the intermediate film.

[0044] In the interlayer having the above configuration A, the minimum thickness (X μm) of the first layer is preferably 130 μm or more, more preferably 140 μm or more, even more preferably 150 μm or more, preferably 300 μm or less, more preferably 290 μm or less, more preferably 280 μm or less, more preferably 270 μm or less, more preferably 260 μm or less, more preferably 250 μm or less, more preferably 240 μm or less, more preferably 230 μm or less, more preferably 220 μm or less, more preferably 210 μm or less, more preferably 200 μm or less, more preferably 190 μm or less, more preferably 180 μm or less, even more preferably 170 μm or less, and particularly preferably 160 μm or less. When the minimum thickness (X μm) is above the lower limit and below the upper limit, the effects of the present invention can be exhibited more effectively, and in particular, the sound insulation performance in the mid-frequency range can be further improved. The minimum thickness (X μm) of the first layer described above may be 125 μm or more, 150 μm or more, 175 μm or more, or 200 μm or more. The minimum thickness (X μm) of the first layer described above may be 200 μm or less, 175 μm or less, or 150 μm or less.

[0045] In the interlayer having the above configuration A, the content of plasticizer in the interlayer (Y parts by weight) relative to 100 parts by weight of thermoplastic resin in the interlayer is preferably 40.5 parts by weight or more, more preferably 41 parts by weight or more, even more preferably 41.5 parts by weight or more, preferably 43.5 parts by weight or less, even more preferably 43 parts by weight or less, even more preferably 42.5 parts by weight or less, and particularly preferably 42 parts by weight or less. When the content of plasticizer (Y parts by weight) is above the lower limit and below the upper limit, the effects of the present invention can be exhibited even more effectively.

[0046] In the intermediate film provided with the above-described Configuration B, X is 125 or more and 250 or less. That is, in the intermediate film provided with the above-described Configuration B, the minimum thickness of the first layer is 125 μm or more and 250 μm or less. Further, the intermediate film provided with the above-described Configuration B satisfies the formula: “−0.0076X + 42.054 ≤ Y ≤ −0.0096X + 45.330”. In the intermediate film provided with the above-described Configuration B, since the minimum thickness of the first layer is relatively thick, the resonance frequency of the laminated glass can be appropriately reduced. Further, in the intermediate film provided with the above-described Configuration B, the relationship between the minimum thickness of the first layer and the content of the plasticizer in the intermediate film is controlled so as to satisfy a specific relational expression. In the intermediate film provided with the above-described Configuration B, the effects of the present invention can be exhibited by controlling the relationship between the minimum thickness of the first layer and the content of the plasticizer in the intermediate film.

[0047] In the intermediate film provided with the above-described Configuration B, the minimum thickness (X μm) of the first layer is preferably 130 μm or more, more preferably 140 μm or more, still more preferably 150 μm or more, preferably 240 μm or less, more preferably 230 μm or less, more preferably 220 μm or less, more preferably 210 μm or less, more preferably 200 μm or less, more preferably 190 μm or less, more preferably 180 μm or less, still more preferably 170 μm or less, particularly preferably 160 μm or less. When the minimum thickness (X μm) is above the lower limit and below the upper limit, the effects of the present invention can be more effectively exhibited. In particular, the sound insulation property in the mid-frequency region can be further enhanced. The minimum thickness (X μm) of the first layer may be 125 μm or more, may be 150 μm or more, may be 175 μm or more, or may be 200 μm or more. The minimum thickness (X μm) of the first layer may be 200 μm or less, may be 175 μm or less, or may be 150 μm or less.

[0048] In the interlayer having the above configuration C, X is 125 or more and 250 or less. That is, in the interlayer having the above configuration C, the minimum thickness of the first layer is 125 μm or more and 250 μm or less. Also, in the interlayer having the above configuration C, Z is 125 or more and 140 or less. That is, in the interlayer having the above configuration C, the primary resonance frequency of the laminated glass G is 125 Hz or more and 140 Hz or less. In the interlayer having the above configuration C, the effects of the present invention can be achieved by controlling both the minimum thickness of the first layer and the primary resonance frequency of the laminated glass G.

[0049] In the interlayer having the above configuration C, the minimum thickness (X μm) of the first layer is preferably 130 μm or more, more preferably 140 μm or more, even more preferably 150 μm or more, preferably 240 μm or less, more preferably 230 μm or less, more preferably 220 μm or less, more preferably 210 μm or less, more preferably 200 μm or less, more preferably 190 μm or less, more preferably 180 μm or less, even more preferably 170 μm or less, and particularly preferably 160 μm or less. When the minimum thickness (X μm) is above the lower limit and below the upper limit, the effects of the present invention can be exhibited more effectively, and in particular, the sound insulation in the mid-frequency range can be further improved. The minimum thickness (X μm) of the first layer may be 125 μm or more, 150 μm or more, 175 μm or more, or 200 μm or more. The minimum thickness (X μm) of the first layer described above may be 200 μm or less, 175 μm or less, or 150 μm or less.

[0050] In the interlayer having the above configuration C, the primary resonant frequency (ZHz) of the laminated glass G is preferably 130 Hz or higher, and preferably 135 Hz or lower. When the primary resonant frequency (ZHz) is above the lower limit and below the upper limit, the effects of the present invention can be exhibited even more effectively. The primary resonant frequency (ZHz) of the laminated glass G may be 126 Hz or higher, 128 Hz or higher, 130 Hz or higher, 133 Hz or higher, 134 Hz ​​or higher, 136 Hz or higher, or 138 Hz or higher. The primary resonant frequency (ZHz) of the laminated glass G may be 138 Hz or lower, 136 Hz or lower, 134 Hz ​​or lower, 133 Hz or lower, 130 Hz or lower, 128 Hz or lower, or 126 Hz or lower.

[0051] In an interlayer comprising at least one of the above configurations A and B, the primary resonant frequency (ZHz) of the laminated glass G may be 117 Hz or higher, 120 Hz or higher, 144 Hz or lower, or 143 Hz or lower.

[0052] The laminated glass G described above is manufactured by placing the interlayer between two sheets of clear glass, each sheet having a thickness of 2.1 mm. The laminated glass G described above is manufactured for measuring the primary resonant frequency. The laminated glass G described above is preferably manufactured as follows.

[0053] Two sheets of clear glass measuring 25 mm in width, 300 mm in length, and 2.1 mm in thickness, conforming to JIS R3202:1996, are prepared. An interlayer measuring 25 mm in width and 300 mm in length is prepared. The interlayer is sandwiched between the two sheets of clear glass to obtain a laminate. The obtained laminate is placed in a rubber bag, degassed at a vacuum of 2.6 kPa for 20 minutes, then transferred to an oven while still degassed, and vacuum-pressed at 90°C for 30 minutes to pre-compress the laminate. The pre-compressed laminate is pressed in an autoclave at 135°C and a pressure of 1.2 MPa for 20 minutes to obtain laminated glass G.

[0054] Furthermore, when manufacturing the laminated glass G, it is preferable that the interlayer, which has a width of 25 mm and a length of 300 mm, includes the minimum thickness portion of the interlayer.

[0055] The primary resonance frequency of the laminated glass G described above is measured as follows.

[0056] Laminated glass G is stored for four weeks at a temperature of 23±2°C and a humidity of 25±5%. After storage, laminated glass G is excited in a constant temperature chamber at 20°C using a vibration generator for damping tests (e.g., Spectris "Pertable Vibration Exciter Type 4809"). The obtained vibration characteristics are amplified using a mechanical impedance measuring device (e.g., Spectris "75 VA Power Amplifier Type 2718"), and the first resonant frequency is determined by FFT analysis of the vibration spectrum. For analysis software, for example, Spectris "PULSE LabShop" can be used.

[0057] Furthermore, when manufacturing laminated glass products using the interlayer film of the present invention, clear glass other than 2.1 mm thick clear glass may be used as the laminated glass member, or laminated glass members other than clear glass may be used.

[0058] The following methods can be used to control the primary resonance frequency of laminated glass G within the above range: (1) Increasing the content of plasticizer in the interlayer (Y parts by weight) relative to 100 parts by weight of thermoplastic resin in the interlayer can reduce the primary resonance frequency. (2) Increasing the minimum thickness (X μm) of the first layer can reduce the primary resonance frequency. (3) Increasing the amount of acetal groups and acetyl groups in the polyvinyl acetal resin in the first layer can reduce the primary resonance frequency. (4) Decreasing the amount of acetal groups and acetyl groups in the polyvinyl acetal resin in the second and third layers can reduce the primary resonance frequency. By appropriately combining these methods, the primary resonance frequency of laminated glass G can be controlled within the above range.

[0059] Specific embodiments of the present invention will be described below with reference to the drawings.

[0060] Figure 1 is a schematic cross-sectional view showing an interlayer for laminated glass according to one embodiment of the present invention.

[0061] Figure 1 is a cross-sectional view along the thickness direction of the interlayer 11. The interlayer 11 comprises a first layer 1, a second layer 2, and a third layer 3. The interlayer 11 has a three-layer structure. The second layer 2 is located on the first surface 1a side of the first layer 1 and is laminated. The third layer 3 is located on the second surface 1b side of the first layer 1, opposite to the first surface 1a, and is laminated. The first layer is an intermediate layer. The second layer 2 and the third layer 3 are protective layers and, in this embodiment, surface layers. The first layer 1 is located between the second layer 2 and the third layer 3 and is sandwiched between them. Therefore, the interlayer 11 has a multilayer structure (second layer 2 / first layer 1 / third layer 3) in which the second layer 2, the first layer 1, and the third layer 3 are laminated in this order.

[0062] Furthermore, other layers may be arranged on the surface of the second layer 2 opposite to the first layer 1, and on the surface of the third layer 3 opposite to the first layer 1.

[0063] The details of the interlayer, the first layer, the second layer, and the third layer according to the present invention, as well as the components used in the interlayer, will be described below.

[0064] <Thermoplastic Resin> The above interlayer contains a thermoplastic resin (hereinafter sometimes referred to as thermoplastic resin (0)). Preferably, the above interlayer contains polyvinyl acetal resin (hereinafter sometimes referred to as polyvinyl acetal resin (0)) as thermoplastic resin (0). Preferably, the above first layer contains a thermoplastic resin (hereinafter sometimes referred to as thermoplastic resin (1)). Preferably, the above first layer contains polyvinyl acetal resin (hereinafter sometimes referred to as polyvinyl acetal resin (1)) as thermoplastic resin (1). Preferably, the thermoplastic resin in the above first layer is polyvinyl acetal resin. Preferably, the above second layer contains a thermoplastic resin (hereinafter sometimes referred to as thermoplastic resin (2)). Preferably, the above second layer contains polyvinyl acetal resin (hereinafter sometimes referred to as polyvinyl acetal resin (2)) as thermoplastic resin (2). Preferably, the thermoplastic resin in the above second layer is polyvinyl acetal resin. The third layer described above preferably contains a thermoplastic resin (hereinafter sometimes referred to as thermoplastic resin (3)). The third layer described above preferably contains polyvinyl acetal resin (hereinafter sometimes referred to as polyvinyl acetal resin (3)) as the thermoplastic resin (3). The thermoplastic resin in the third layer described above preferably is polyvinyl acetal resin. The thermoplastic resin (1), the thermoplastic resin (2), and the thermoplastic resin (3) described above may be the same or different. It is preferable that the thermoplastic resin (1) is different from the thermoplastic resin (2) and the thermoplastic resin (3) described above in order to further improve sound insulation. The polyvinyl acetal resin (1), the polyvinyl acetal resin (2), and the polyvinyl acetal resin (3) described above may be the same or different. It is preferable that the polyvinyl acetal resin (1) is different from the polyvinyl acetal resin (2) and the polyvinyl acetal resin (3) described above in order to further improve sound insulation. The thermoplastic resin (0), thermoplastic resin (1), thermoplastic resin (2), and thermoplastic resin (3) may each be used individually or in combination of two or more types.The polyvinyl acetal resin (0), polyvinyl acetal resin (1), polyvinyl acetal resin (2), and polyvinyl acetal resin (3) may be used individually or in combination of two or more types.

[0065] In the following description, the common components of the thermoplastic resin (0), thermoplastic resin (1), thermoplastic resin (2), and thermoplastic resin (3) will be simply referred to as "thermoplastic resin."

[0066] Examples of the thermoplastic resins mentioned above include polyvinyl acetal resin, ethylene-vinyl acetate copolymer resin, ethylene-acrylic acid copolymer resin, polyurethane resin, (meth)acrylic resin, polyolefin resin, ionomer resin, and polyvinyl alcohol resin. Other thermoplastic resins may also be used.

[0067] The above-mentioned polyvinyl acetal resin can be produced, for example, by acetalizing polyvinyl alcohol (PVA) with an aldehyde. Preferably, the polyvinyl acetal resin is 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 mol% to 99.9 mol%.

[0068] The average degree of polymerization of the polyvinyl alcohol (PVA) is preferably 200 or higher, more preferably 500 or higher, even more preferably 1500 or higher, still more preferably 1600 or higher, particularly preferably 2600 or higher, most preferably 2700 or higher, preferably 5000 or lower, more preferably 4000 or lower, and still more preferably 3500 or lower. If the average degree of polymerization is above the lower limit, the penetration resistance of the laminated glass is further increased. If the average degree of polymerization is below the upper limit, the molding of the interlayer film becomes easier.

[0069] The average degree of polymerization of the above polyvinyl alcohol is determined by a method in accordance with JIS K6726 "Test Method for Polyvinyl Alcohol".

[0070] The number of carbon atoms in the acetal group contained in the above polyvinyl acetal resin is not particularly limited. The aldehyde used in the production of the above polyvinyl acetal resin is not particularly limited. The number of carbon atoms in the acetal group in the above polyvinyl acetal resin is preferably 3 to 5, and more preferably 3 or 4. When the number of carbon atoms in the acetal group in the above polyvinyl acetal resin is 3 or more, the glass transition temperature of the interlayer becomes sufficiently low. The number of carbon atoms in the acetal group in the above polyvinyl acetal resin may be 4 or 5.

[0071] Generally, aldehydes having 1 to 10 carbon atoms are preferred as the above-mentioned aldehyde. Examples of aldehydes having 1 to 10 carbon atoms include propionaldehyde, n-butyraldehyde, isobutyraldehyde, n-valeraldehyde, 2-ethylbutyraldehyde, n-hexylaldehyde, n-octylaldehyde, n-nonylaldehyde, n-decylaldehyde, formaldehyde, acetaldehyde, and benzaldehyde. The above-mentioned aldehyde is preferably propionaldehyde, n-butyraldehyde, isobutyraldehyde, n-hexylaldehyde, or n-valeraldehyde, more preferably propionaldehyde, n-butyraldehyde, or isobutyraldehyde, and even more preferably n-butyraldehyde. The above-mentioned aldehydes may be used individually or in combination of two or more.

[0072] The polyvinyl acetal resin (0) is preferably polyvinyl butyral resin. The polyvinyl acetal resin (1) is preferably polyvinyl butyral resin. The polyvinyl acetal resin (2) is preferably polyvinyl butyral resin. The polyvinyl acetal resin (3) is preferably polyvinyl butyral resin.

[0073] The hydroxyl group content (amount of hydroxyl groups) of the polyvinyl acetal resin (0) is preferably 15 mol% or more, more preferably 18 mol% or more, preferably 40 mol% or less, and more preferably 35 mol% or less. If the hydroxyl group content is above the lower limit, the adhesive strength of the interlayer film is further increased. If the hydroxyl group content is below the upper limit, the flexibility of the interlayer film is increased, making it easier to handle.

[0074] The hydroxyl group content (amount of hydroxyl groups) of the polyvinyl acetal resin (1) is preferably 17 mol% or more, more preferably 20 mol% or more, even more preferably 22 mol% or more, preferably 28 mol% or less, more preferably 27 mol% or less, even more preferably 25 mol% or less, and particularly preferably 24 mol% or less. When the hydroxyl group content is above 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 productivity is excellent, and when it is 28 mol% or less, the sound insulation of the laminated glass is further increased. Furthermore, when the hydroxyl group content is below the upper limit, the flexibility of the interlayer film is increased and the handling of the interlayer film becomes easier.

[0075] The hydroxyl group content (amount of hydroxyl groups) of 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, even more preferably 31.5 mol% or more, even more preferably 32 mol% or more, particularly preferably 33 mol% or more, preferably 38 mol% or less, more preferably 37 mol% or less, even more preferably 36.5 mol% or less, and particularly preferably 36 mol% or less. When the hydroxyl group content is above the lower limit, the adhesive strength of the interlayer film is further increased. Also, when the hydroxyl group content is below the upper limit, the flexibility of the interlayer film is increased, making it easier to handle.

[0076] From the viewpoint of further improving sound insulation, it is preferable that the hydroxyl group content of the polyvinyl acetal resin (1) is lower than the hydroxyl group content of the polyvinyl acetal resin (2). From the viewpoint of further improving sound insulation, it is preferable that the hydroxyl group content of the polyvinyl acetal resin (1) is lower than the hydroxyl group content of the polyvinyl acetal resin (3). The absolute value of the difference between the hydroxyl group content of the polyvinyl acetal resin (1) and the hydroxyl group content of the polyvinyl acetal resin (2) is denoted as absolute value A, and the absolute value of the difference between the hydroxyl group content of the polyvinyl acetal resin (1) and the hydroxyl group content of the polyvinyl acetal resin (3) is denoted as absolute value B. From the viewpoint of further improving sound insulation, absolute values ​​A and B are preferably 1 mol% or more, more preferably 5 mol% or more, even more preferably 9 mol% or more, particularly preferably 10 mol% or more, and most preferably 12 mol% or more. The absolute values ​​A and B are preferably 20 mol% or less, respectively.

[0077] The degree of acetylation (amount of acetyl groups) of the above polyvinyl acetal resin (0) is preferably 0.1 mol% or more, more preferably 0.3 mol% or more, even more preferably 0.5 mol% or more, preferably 30 mol% or less, more preferably 25 mol% or less, and even more preferably 20 mol% or less. When the degree of acetylation is above the lower limit, the compatibility between the polyvinyl acetal resin and the plasticizer is high. When the degree of acetylation is below the upper limit, the moisture resistance of the interlayer and laminated glass is high.

[0078] The degree of acetylation (amount of acetyl groups) of the polyvinyl acetal resin (1) is preferably 0.01 mol% or more, more preferably 0.1 mol% or more, even more preferably 7 mol% or more, even more preferably 9 mol% or more, preferably 30 mol% or less, more preferably 25 mol% or less, even more preferably 24 mol% or less, and particularly preferably 20 mol% or less. When the degree of acetylation is above the lower limit, the compatibility between the polyvinyl acetal resin and the plasticizer is high. When the degree of acetylation is below the upper limit, the moisture resistance of the interlayer and laminated glass is high. In particular, when the degree of acetylation of the polyvinyl acetal resin (1) is 0.1 mol% or more and 25 mol% or less, the puncture resistance is excellent.

[0079] The degree of acetylation (amount of acetyl groups) 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, and more preferably 2 mol% or less. When the degree of acetylation is above the lower limit, the compatibility between the polyvinyl acetal resin and the plasticizer is high. When the degree of acetylation is below the upper limit, the moisture resistance of the interlayer and the laminated glass is high.

[0080] The degree of acetylation described above is a value expressed as a percentage of the mole fraction obtained by dividing the amount of ethylene groups to which acetyl groups are attached by the total amount of ethylene groups in the main chain. The amount of ethylene groups to which acetyl groups are attached can be measured, for example, in accordance with JIS K6728 "Test Method for Polyvinyl Butyral".

[0081] The degree of acetalization of the above polyvinyl acetal resin (0) (or the degree of butyralization in the case of polyvinyl butyral resin) is preferably 60 mol% or more, more preferably 63 mol% or more, preferably 85 mol% or less, more preferably 75 mol% or less, and even more preferably 70 mol% or less. When the degree of acetalization is above the lower limit, the compatibility between the polyvinyl acetal resin and the plasticizer is increased. When the degree of acetalization is below the upper limit, the reaction time required to produce the polyvinyl acetal resin is shortened.

[0082] The degree of acetalization of the above polyvinyl acetal resin (1) (or the degree of butyralization in the case of polyvinyl butyral resin) is preferably 47 mol% or more, more preferably 60 mol% or more, preferably 85 mol% or less, more preferably 80 mol% or less, and even more preferably 75 mol% or less. When the degree of acetalization is above the lower limit, the compatibility between the polyvinyl acetal resin and the plasticizer is increased. When the degree of acetalization is below the upper limit, the reaction time required to produce the polyvinyl acetal resin is shortened.

[0083] The degree of acetalization of the polyvinyl acetal resin (2) and the polyvinyl acetal resin (3) (or the degree of butyralization in the case of polyvinyl butyral resin) is preferably 55 mol% or more, more preferably 60 mol% or more, preferably 75 mol% or less, and more preferably 71 mol% or less. When the degree of acetalization is above the lower limit, the compatibility between the polyvinyl acetal resin and the plasticizer is increased. When the degree of acetalization is below the upper limit, the reaction time required to produce the polyvinyl acetal resin is shortened.

[0084] The degree of acetalization (or butyralization in the case of polyvinyl butyral resin), acetylation, and hydroxyl group content of polyvinyl acetal resin can be determined by measuring them under the following conditions using a nuclear magnetic resonance spectrometer (for example, a Bruker Ascend 400). For analysis software, for example, JEOL Delta can be used.

[0085] <Measurement Conditions> Measurement temperature: 80°C Number of cumulative measurements: 64 times / D1 = 1 sec H-NMR standard conditions (1H45Z) Measurement solvent: DMSO Resin concentration: 1% by weight

[0086] From the obtained spectrum, the following integral values ​​B to E are calculated. If the edges of the detected peaks overlap, the minimum value between each peak is used as the delimiter for the integral value.

[0087] Integrated value B: Integrated value of peak B (peak detected between 2.00 ppm and 2.30 ppm) Integrated value C: Integrated value of peak C (peak detected between 1.80 ppm and 2.00 ppm) Integrated value D: Integrated value of peak D (peak detected between 1.00 ppm and 1.80 ppm) Integrated value E: Integrated value of peak E (peak detected between 0.50 ppm and 1.00 ppm)

[0088] The degree of acetalization, degree of acetylation, and hydroxyl group content are calculated from the obtained integral values ​​using the following formulas. In the following formulas, B to E are the integral values ​​B to E mentioned above, respectively.

[0089] Acetalization degree (mol%) = (4 / 3 × E) ÷ (B + D - 4 / 3 × E) × 100

[0090] Degree of acetylation (mol%) = (2 / 3 × C) ÷ (B + D - 4 / 3 × E) × 100

[0091] Hydroxyl group content (mol%) = 100 - (4 / 3 × E + 2 / 3 × C) ÷ (B + D - 4 / 3 × E) × 100

[0092] In the above-mentioned interlayer film, the content of polyvinyl acetal resin in 100% by weight of thermoplastic resin is preferably 10% by weight or more, more preferably 30% by weight or more, even more preferably 50% by weight or more, even more preferably 70% by weight or more, particularly preferably 80% by weight or more, most preferably 90% by weight or more, and preferably 100% by weight or less. The main component (50% by weight or more) of the thermoplastic resin in the above-mentioned interlayer film is preferably polyvinyl acetal resin.

[0093] In the first layer described above, the content of polyvinyl acetal resin in 100% by weight of thermoplastic resin is preferably 10% by weight or more, more preferably 30% by weight or more, even more preferably 50% by weight or more, still more preferably 70% by weight or more, particularly preferably 80% by weight or more, most preferably 90% by weight or more, and preferably 100% by weight or less. The main component (50% by weight or more) of the thermoplastic resin in the first layer described above is preferably polyvinyl acetal resin.

[0094] In the second layer, the content of polyvinyl acetal resin in 100% by weight of thermoplastic resin is preferably 10% by weight or more, more preferably 30% by weight or more, even more preferably 50% by weight or more, still more preferably 70% by weight or more, particularly preferably 80% by weight or more, most preferably 90% by weight or more, and preferably 100% by weight or less. The main component (50% by weight or more) of the thermoplastic resin in the second layer is preferably polyvinyl acetal resin.

[0095] In the third layer described above, the content of polyvinyl acetal resin in 100% by weight of thermoplastic resin is preferably 10% by weight or more, more preferably 30% by weight or more, even more preferably 50% by weight or more, still more preferably 70% by weight or more, particularly preferably 80% by weight or more, most preferably 90% by weight or more, and preferably 100% by weight or less. The main component (50% by weight or more) of the thermoplastic resin in the third layer described above is preferably polyvinyl acetal resin.

[0096] <Plasticizer> The above interlayer contains a plasticizer (hereinafter sometimes referred to as plasticizer (0)). The above first layer preferably contains a plasticizer (hereinafter sometimes referred to as plasticizer (1)). The above second layer preferably contains a plasticizer (hereinafter sometimes referred to as plasticizer (2)). The above third layer preferably contains a plasticizer (hereinafter sometimes referred to as plasticizer (3)). When the thermoplastic resin contained in the interlayer is polyvinyl acetal resin, it is particularly preferable that the interlayer (each layer) contains a plasticizer. The layer containing polyvinyl acetal resin preferably contains a plasticizer.

[0097] In the following description, the common components of plasticizer (0), plasticizer (1), plasticizer (2), and plasticizer (3) will be simply referred to as "plasticizer."

[0098] The plasticizer described above is not particularly limited. Conventionally known plasticizers can be used as the plasticizer. Only one type of plasticizer may be used, or two or more types may be used in combination.

[0099] Examples of the above-mentioned plasticizers include organic ester plasticizers such as monobasic organic acid esters and polybasic organic acid esters, organic phosphate plasticizers, and organic phosphite plasticizers. The above-mentioned plasticizer is preferably an organic ester plasticizer. The above-mentioned plasticizer is preferably a liquid plasticizer.

[0100] Examples of the monobasic organic acid esters mentioned above include glycol esters obtained by the reaction of glycol with a monobasic organic acid. Examples of the glycols mentioned above include triethylene glycol, tetraethylene glycol, and tripropylene glycol. Examples of the monobasic organic acids mentioned above include butyric acid, isobutyric acid, caproic acid, 2-ethylbutyric acid, heptylic acid, n-octyl acid, 2-ethylhexyl acid, n-nonylic acid, decyl acid, and benzoic acid.

[0101] Examples of the above-mentioned polybasic organic acid esters include ester compounds of a polybasic organic acid and an alcohol having a linear or branched structure with 4 to 8 carbon atoms. Examples of the above-mentioned polybasic organic acids include adipic acid, sebacic acid, and azelaic acid.

[0102] The above organic ester plasticizers 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-ethylbutyrate, 1,4-butylene glycol di-2-ethylbutyrate, and diethylene glycol di-2-ethylbutyrate Examples include diethylene glycol di-2-ethylhexanoate, dipropylene glycol di-2-ethylbutyrate, triethylene glycol di-2-ethylpentanoate, tetraethylene glycol di-2-ethylbutyrate, diethylene glycol dicaprylate, diethylene glycol dibenzoate, dipropylene glycol dibenzoate, dihexyl adipate, dioctyl adipate, hexylcyclohexyl adipate, a mixture of heptyl adipate and nonyl adipate, diisononyl adipate, diisodecyl adipate, heptylnonyl adipate, dibutyl sebacate, oil-modified alkyd sebacate, and a mixture of phosphate esters and adipic acid esters. Other organic ester plasticizers may be used as the above organic ester plasticizers. In addition, other adipic acid esters other than those listed above may be used as the adipic acid ester.

[0103] Examples of the above-mentioned organic phosphate plasticizers include tributoxyethyl phosphate, isodecylphenyl phosphate, and triisopropyl phosphate.

[0104] The above plasticizer is preferably a diester plasticizer represented by the following formula (1).

[0105]

[0106] In formula (1) above, R1 and R2 each represent an organic group having 2 to 10 carbon atoms, R3 represents an ethylene group, an isopropylene group, or an n-propylene group, and p represents an integer from 3 to 10. Preferably, R1 and R2 in formula (1) above are organic groups having 5 to 10 carbon atoms, and more preferably are organic groups having 6 to 10 carbon atoms.

[0107] The above plasticizer preferably contains triethylene glycol di-2-ethylhexanoate (3GO), triethylene glycol di-2-ethyl butyrate (3GH), or triethylene glycol di-2-ethylpropanoate. The above plasticizer more preferably contains triethylene glycol di-2-ethylhexanoate (3GO) or triethylene glycol di-2-ethyl butyrate (3GH), and even more preferably contains triethylene glycol di-2-ethylhexanoate (3GO).

[0108] The content of the plasticizer (0) in the interlayer film relative to 100 parts by weight of the thermoplastic resin (0) is defined as content (0). The content (0) is the content (Y parts by weight) of the plasticizer in the interlayer film relative to 100 parts by weight of the thermoplastic resin in the interlayer film. The content (0) is preferably 5 parts by weight or more, more preferably 25 parts by weight or more, even more preferably 30 parts by weight or more, preferably 100 parts by weight or less, more preferably 60 parts by weight or less, and even more preferably 50 parts by weight or less. If the content (0) is above the lower limit, the penetration resistance of the laminated glass is further increased. If the content (0) is below the upper limit, the transparency of the interlayer film is further increased. The content (0) may be 40 parts by weight or more, or 44 parts by weight or less. In the interlayer film having the above configuration A, the content (0) is 40 parts by weight or more and 44 parts by weight or less. The above content (0) may be 40.2 parts by weight or more, 40.5 parts by weight or more, 40.7 parts by weight or more, 41.0 parts by weight or more, 41.4 parts by weight or more, 41.6 parts by weight or more, 41.7 parts by weight or more, 42.8 parts by weight or more, 43.0 parts by weight or more, or 43.4 parts by weight or more. The above content (0) may be 43.4 parts by weight or less, 43.0 parts by weight or less, 42.8 parts by weight or less, 41.7 parts by weight or less, 41.6 parts by weight or less, 41.4 parts by weight or less, 41.0 parts by weight or less, 40.7 parts by weight or less, 40.5 parts by weight or less, or 40.2 parts by weight or less.

[0109] The content of the plasticizer (1) in the first layer relative to 100 parts by weight of the thermoplastic resin (1) in the first layer shall be defined as content (1). The content of the plasticizer (2) in the second layer relative to 100 parts by weight of the thermoplastic resin (2) in the second layer shall be defined as content (2). The content of the plasticizer (3) in the third layer relative to 100 parts by weight of the thermoplastic resin (3) in the third layer shall be defined as content (3).

[0110] The amount of (1) is preferably greater than the amount of (2), and the amount of (1) is preferably greater than the amount of (3). In this case, the sound insulation in the mid-frequency range can be further improved.

[0111] The absolute value of the difference between the above content (1) and the above content (2) is preferably 20 parts by weight or more, more preferably 30 parts by weight or more, even more preferably 40 parts by weight or more, preferably 70 parts by weight or less, more preferably 60 parts by weight or less, and even more preferably 50 parts by weight or less. If the absolute value of the above difference is above the lower limit and below the upper limit, the sound insulation in the mid-frequency range can be further improved.

[0112] The above content (1) is preferably 50 parts by weight or more, more preferably 60 parts by weight or more, even more preferably 70 parts by weight or more, preferably 100 parts by weight or less, more preferably 90 parts by weight or less, and even more preferably 80 parts by weight or less. When the above content (1) is above the lower limit and below the upper limit, the sound insulation performance in the mid-frequency range can be further improved. When the above content (1) is above the lower limit, the flexibility of the interlayer increases, making the interlayer easier to handle. When the above content (1) is below the upper limit, the penetration resistance of the laminated glass is further improved.

[0113] The above content (2) is preferably 5 parts by weight or more, more preferably 10 parts by weight or more, even 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, most preferably 25 parts by weight or more, preferably 45 parts by weight or less, more preferably 40 parts by weight or less, still more preferably 35 parts by weight or less, particularly preferably 32 parts by weight or less, and most preferably 30 parts by weight or less. If the above content (2) is above the lower limit, the flexibility of the interlayer film increases, making it easier to handle the interlayer film. If the above content (2) is below the upper limit, the penetration resistance of the laminated glass increases even further.

[0114] The above content (3) is preferably 5 parts by weight or more, more preferably 10 parts by weight or more, even 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, most preferably 25 parts by weight or more, preferably 45 parts by weight or less, more preferably 40 parts by weight or less, still more preferably 35 parts by weight or less, particularly preferably 32 parts by weight or less, and most preferably 30 parts by weight or less. If the above content (3) is above the lower limit, the flexibility of the interlayer film increases and the handling of the interlayer film becomes easier. If the above content (3) is below the upper limit, the penetration resistance of the laminated glass becomes even higher.

[0115] <Heat-shielding substance> The above interlayer preferably contains a heat-shielding substance. The above first layer preferably contains a heat-shielding substance. The above second layer preferably contains a heat-shielding substance. The above third layer preferably contains a heat-shielding substance. Only one type of heat-shielding substance may be used, or two or more types may be used in combination.

[0116] The heat-shielding substance preferably contains at least one component X from among phthalocyanine compounds, naphthalocyanine compounds, and anthracianine compounds, or it may contain heat-shielding particles. In this case, the heat-shielding substance may contain both component X and the heat-shielding particles. That is, the heat-shielding substance preferably contains at least one component from among phthalocyanine compounds, naphthalocyanine compounds, anthracianine compounds, and heat-shielding particles.

[0117] Component X: The interlayer preferably contains at least one component X selected from phthalocyanine compounds, naphthalocyanine compounds, and anthracianine compounds. The first layer preferably contains component X. The second layer preferably contains component X. The third layer preferably contains component X. Component X is a heat-shielding substance. Only one type of component X may be used, or two or more types may be used in combination.

[0118] The above-mentioned component X is not particularly limited. Conventionally known phthalocyanine compounds, naphthalocyanine compounds, and anthracianine compounds can be used as component X.

[0119] Examples of component X include phthalocyanine, phthalocyanine derivatives, naphthalocyanine, naphthalocyanine derivatives, anthracianine, and anthracianine derivatives. It is preferable that the phthalocyanine compound and the phthalocyanine derivative each have a phthalocyanine skeleton. It is preferable that the naphthalocyanine compound and the naphthalocyanine derivative each have a naphthalocyanine skeleton. It is preferable that the anthracianine compound and the anthracianine derivative each have an anthracianine skeleton.

[0120] From the viewpoint of further improving heat shielding properties, it is preferable that component X is at least one selected from the group consisting of phthalocyanine, phthalocyanine derivatives, naphthalocyanine, and naphthalocyanine derivatives, and more preferably at least one of phthalocyanine and phthalocyanine derivatives.

[0121] From the viewpoint of effectively enhancing heat shielding properties and maintaining a higher level of visible light transmittance over a long period of time, it is preferable that component X contains a vanadium atom or a copper atom. It is preferable that component X contains a vanadium atom, and it is also preferable that it contains a copper atom. It is more preferable that component X is at least one of phthalocyanine containing a vanadium atom or a copper atom, and a derivative of phthalocyanine containing a vanadium atom or a copper atom. From the viewpoint of further enhancing heat shielding properties, it is preferable that component X has a structural unit in which an oxygen atom is bonded to a vanadium atom.

[0122] In 100% by weight of the above-mentioned interlayer film or in 100% by weight of the layer containing the above-mentioned component X (first layer, second layer, or third layer), the content of component X is preferably 0.001% by weight or more, more preferably 0.005% by weight or more, even more preferably 0.01% by weight or more, particularly preferably 0.02% by weight or more, preferably 0.2% by weight or less, more preferably 0.1% by weight or less, even more preferably 0.05% by weight or less, and particularly preferably 0.04% by weight or less. When the content of component X is above the lower limit and below the upper limit, the heat shielding performance becomes sufficiently high and the visible light transmittance becomes sufficiently high. For example, it is possible to make the visible light transmittance 70% or more.

[0123] Heat-shielding particles: The interlayer preferably contains heat-shielding particles. The first layer preferably contains heat-shielding particles. The second layer preferably contains heat-shielding particles. The third layer preferably contains heat-shielding particles. The heat-shielding particles are heat-shielding materials. By using heat-shielding particles, infrared rays (heat rays) can be effectively blocked. Only one type of heat-shielding particle may be used, or two or more types may be used in combination.

[0124] From the viewpoint of further enhancing heat shielding performance, it is preferable that the heat shielding particles are metal oxide particles. It is preferable that the heat shielding particles are particles formed from metal oxides (metal oxide particles).

[0125] Infrared rays with wavelengths longer than visible light (780 nm and above) have less energy than ultraviolet rays. However, infrared rays have a strong thermal effect, and when they are absorbed by a substance, they are emitted as heat. For this reason, infrared rays are generally called heat rays. By using the heat-shielding particles mentioned above, infrared rays (heat rays) can be effectively blocked. Note that heat-shielding particles refer to particles that can absorb infrared rays.

[0126] Specific examples of the above heat-shielding particles include metal oxide particles such as aluminum-doped tin oxide particles, indium-doped tin oxide particles, antimond-doped tin oxide particles (ATO particles), gallium-doped zinc oxide particles (GZO particles), 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), tin-doped zinc oxide particles, silicon-doped zinc oxide particles, and lanthanum hexaboride (LaB ６ Examples include particles such as ) and others. Other heat-shielding particles may also be used. Metal oxide particles are preferred because they have a high heat-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 preferred because they have a high heat-shielding function and are readily available, and tungsten oxide particles are also preferred.

[0127] From the viewpoint of further improving heat shielding performance, it is preferable that the tungsten oxide particles are metal-doped tungsten oxide particles. The above-mentioned "tungsten oxide particles" include metal-doped tungsten oxide particles. Specifically, examples of the above-mentioned 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.

[0128] From the viewpoint of further improving heat shielding performance, cesium-doped tungsten oxide particles are particularly preferred. From the viewpoint of further improving heat shielding performance, the cesium-doped tungsten oxide particles are of the formula: Cs ０．３３ WO ３ Preferably, the particles are tungsten oxide particles represented by [formula].

[0129] 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, and more preferably 0.05 μm or less. If the average particle diameter is above the lower limit, the heat-shielding performance becomes sufficiently high. If the average particle diameter is below the upper limit, the dispersibility of the heat-shielding particles becomes high.

[0130] The "average particle diameter" mentioned above refers to the volume-average particle diameter. The average particle diameter can be measured using a particle size distribution analyzer (such as the "UPA-EX150" manufactured by Nikkiso Co., Ltd.).

[0131] In 100% by weight of the above-mentioned interlayer film or in 100% by weight of the layer containing the above-mentioned heat-shielding particles (first layer, second layer, or third layer), the content of the heat-shielding particles (particularly the content of tungsten oxide particles) is preferably 0.01% by weight or more, more preferably 0.1% by weight or more, even more preferably 1% by weight or more, particularly preferably 1.5% by weight or more, preferably 6% by weight or less, more preferably 5.5% by weight or less, even more 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 above-mentioned heat-shielding particles is above the lower limit and below the upper limit, the heat-shielding performance becomes sufficiently high and the visible light transmittance becomes sufficiently high.

[0132] <Metal Salts> The interlayer preferably contains at least one metal salt (hereinafter sometimes referred to as metal salt M) from among alkali metal salts and alkaline earth metal salts. The first layer preferably contains metal salt M. The second layer preferably contains metal salt M. The third layer preferably contains metal salt M. Alkaline earth metals refer to the six metals Be, Mg, Ca, Sr, Ba, and Ra. The use of metal salt M makes it easy to control the adhesion between the interlayer and the laminated glass member such as a glass plate, or the adhesion between each layer in the interlayer. Only one type of metal salt M may be used, or two or more types may be used in combination.

[0133] The above metal salt M preferably contains at least one metal selected from the group consisting of Li, Na, K, Rb, Cs, Mg, Ca, Sr, and Ba. The metal salt M contained in the interlayer preferably contains at least one metal from K and Mg.

[0134] Furthermore, as the metal salt M, alkali metal salts of organic acids having 2 to 16 carbon atoms and alkaline earth metal salts of organic acids having 2 to 16 carbon atoms can be used. The metal salt M may also contain magnesium carboxylate salts having 2 to 16 carbon atoms or potassium carboxylate salts having 2 to 16 carbon atoms.

[0135] Examples of magnesium carboxylate salts having 2 to 16 carbon atoms and potassium carboxylate salts having 2 to 16 carbon atoms include magnesium acetate, potassium acetate, magnesium propionate, potassium propionate, magnesium 2-ethylbutyrate, potassium 2-ethylbutanoate, magnesium 2-ethylhexanoate, and potassium 2-ethylhexanoate.

[0136] The total content of Mg and K in the above-mentioned interlayer or the layer containing the above-mentioned metal salt M (first layer, second layer, or third layer) is preferably 5 ppm or more, more preferably 10 ppm or more, even more preferably 20 ppm or more, preferably 300 ppm or less, more preferably 250 ppm or less, and even more preferably 200 ppm or less. When the total content of Mg and K is above the lower limit and below the upper limit, the adhesion between the interlayer and the laminated glass member (glass plate, etc.) or the adhesion between each layer in the interlayer can be controlled to an even better degree.

[0137] <UV-blocking agent> The interlayer preferably contains a UV-blocking agent. The first layer preferably contains a UV-blocking agent. The second layer preferably contains a UV-blocking agent. The third layer preferably contains a UV-blocking agent. The use of a UV-blocking agent makes it less likely for the visible light transmittance of the laminated glass to decrease even after long-term use. Only one type of UV-blocking agent may be used, or two or more types may be used in combination.

[0138] The above-mentioned UV shielding agent includes a UV absorber. Preferably, the above-mentioned UV shielding agent is a UV absorber.

[0139] Examples of the above-mentioned ultraviolet shielding agents include ultraviolet shielding agents containing metal atoms, ultraviolet shielding agents containing metal oxides, ultraviolet shielding agents having a benzotriazole structure (benzotriazole compounds), ultraviolet shielding agents having a benzophenone structure (benzophenone compounds), ultraviolet shielding agents having a triazine structure (triazine compounds), ultraviolet shielding agents having a malonic acid ester structure (malonic acid ester compounds), ultraviolet shielding agents having an oxalic acid anilide structure (oxalic acid anilide compounds), and ultraviolet shielding agents having a benzoate structure (benzoate compounds).

[0140] Examples of UV shielding agents containing the above-mentioned metal atoms include platinum particles, particles in which the surface of platinum particles is coated with silica, palladium particles, and particles in which the surface of palladium particles is coated with silica. It is preferable that the UV shielding agent is not a heat-shielding particle.

[0141] The above 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 above ultraviolet shielding agent is more preferably an ultraviolet shielding agent having a benzotriazole structure or an ultraviolet shielding agent having a benzophenone structure, and even more preferably an ultraviolet shielding agent having a benzotriazole structure.

[0142] Examples of UV shielding agents containing the above-mentioned metal oxides include zinc oxide, titanium oxide, and cerium oxide. Furthermore, the surface of the UV shielding agent containing the above-mentioned metal oxide may be coated. Examples of coating materials for the surface of the UV shielding agent containing the above-mentioned metal oxides include insulating metal oxides, hydrolyzable organosilicon compounds, and silicone compounds.

[0143] Examples of the above-mentioned insulating metal oxides include silica, alumina, and zirconia. The above-mentioned insulating metal oxides have a band gap energy of, for example, 5.0 eV or more.

[0144] Examples of UV-blocking agents having the above-mentioned benzotriazole structure include 2-(2'-hydroxy-5'-methylphenyl)benzotriazole (BASF's "Tinuvin P"), 2-(2'-hydroxy-3',5'-di-t-butylphenyl)benzotriazole (BASF's "Tinuvin 320"), 2-(2'-hydroxy-3'-t-butyl-5-methylphenyl)-5-chlorobenzotriazole (BASF's "Tinuvin 326"), and 2-(2'-hydroxy-3',5'-diamylphenyl)benzotriazole (BASF's "Tinuvin 328"). Because they exhibit excellent UV-blocking performance, the above-mentioned UV-blocking agents are preferably UV-blocking agents having a benzotriazole structure containing a halogen atom, and more preferably UV-blocking agents having a benzotriazole structure containing a chlorine atom.

[0145] Examples of UV-blocking agents having the above-mentioned benzophenone structure include octabenzone (BASF's "Chimassorb 81").

[0146] Examples of UV shielding agents having the above triazine structure include "LA-F70" manufactured by ADEKA Corporation and 2-(4,6-diphenyl-1,3,5-triazine-2-yl)-5-[(hexyl)oxy]-phenol ("Tinuvin 1577FF" manufactured by BASF Corporation).

[0147] Examples of UV shielding agents having the above-mentioned malonic acid 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-pentamethyl4-piperidinyl)malonate.

[0148] Examples of commercially available UV-blocking agents having the above-mentioned malonic acid ester structure include Hostavin B-CAP, Hostavin PR-25, and Hostavin PR-31 (all manufactured by Clariant).

[0149] Examples of UV shielding agents having the above-mentioned oxalic acid anilide structure include oxalic acid diamides having substituted aryl groups on the nitrogen atom, such as N-(2-ethylphenyl)-N'-(2-ethoxy-5-t-butylphenyl)oxalic acid diamide, N-(2-ethylphenyl)-N'-(2-ethoxy-phenyl)oxalic acid diamide, and 2-ethyl-2'-ethoxy-oxalanilide (Sanduvor VSU, manufactured by Clariant).

[0150] Examples of UV-blocking agents having the above-mentioned benzoate structure include 2,4-di-tert-butylphenyl-3,5-di-tert-butyl-4-hydroxybenzoate (BASF's "Tinuvin 120").

[0151] In 100% by weight of the above-mentioned interlayer or in 100% by weight of the layer containing the above-mentioned ultraviolet shielding agent (first layer, second layer, or third layer), the content of the ultraviolet shielding agent is preferably 0.1% by weight or more, more preferably 0.2% by weight or more, even more preferably 0.3% by weight or more, particularly preferably 0.5% by weight or more, preferably 2.5% by weight or less, more preferably 2% by weight or less, even more preferably 1% by weight or less, and particularly preferably 0.8% by weight or less. If the content of the ultraviolet shielding agent is above the above lower limit, the decrease in visible light transmittance of the interlayer and laminated glass after a period of time is further suppressed. If the content of the ultraviolet shielding agent is below the above upper limit, the decrease in visible light transmittance of the interlayer and laminated glass after a period of time can be significantly suppressed.

[0152] <Antioxidant> The above-mentioned interlayer preferably contains an antioxidant. The above-mentioned first layer preferably contains an antioxidant. The above-mentioned second layer preferably contains an antioxidant. The above-mentioned third layer preferably contains an antioxidant. Only one type of antioxidant may be used, or two or more types may be used in combination.

[0153] Examples of the above-mentioned antioxidants include phenolic antioxidants, sulfuric antioxidants, and phosphorusic antioxidants. The phenolic antioxidant is an antioxidant having a phenol skeleton. The sulfuric antioxidant is an antioxidant containing a sulfur atom. The phosphorusic antioxidant is an antioxidant containing a phosphorus atom.

[0154] The above antioxidant is preferably a phenolic antioxidant or a phosphorus-based antioxidant.

[0155] The above phenolic antioxidants 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), and 1,1,3-tris-(2-methyl-hydroxy-5- Examples include t-butylphenyl)butane, tetrakis[methylene-3-(3',5'-butyl-4-hydroxyphenyl)propionate]methane, 1,3,3-tris-(2-methyl-4-hydroxy-5-t-butylphenol)butane, 1,3,5-trimethyl-2,4,6-tris(3,5-di-t-butyl-4-hydroxybenzyl)benzene, bis(3,3'-t-butylphenol)butyric acid glycol ester, and bis(3-t-butyl-4-hydroxy-5-methylbenzenepropanoic acid)ethylenebis(oxyethylene). One or more of these antioxidants are preferably used.

[0156] Examples of the phosphorus-based antioxidants mentioned above include tridecyl phosphite, tris(tridecyl) phosphite, triphenyl phosphite, trinonylphenyl phosphite, bis(tridecyl)pentaerythritol diphosphite, bis(decyl)pentaerythritol diphosphite, 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. One or more of these antioxidants are preferably used.

[0157] Examples of commercially available antioxidants include BASF's "IRGANOX 245," "IRGAFOS 168," and "IRGAFOS 38," Sumitomo Chemical's "SumiLizer BHT," Sakai Chemical Industry's "H-BHT," and BASF's "IRGANOX 1010."

[0158] In order to maintain the high visible light transmittance of the interlayer and laminated glass over a long period of time, the content of the antioxidant in 100% by weight of the interlayer or in 100% by weight of the layer containing the antioxidant (first layer, second layer, or third layer) is preferably 0.03% by weight or more, and more preferably 0.1% by weight or more. Furthermore, since the effect of adding the antioxidant becomes saturated, the content of the antioxidant in 100% by weight of the interlayer or in 100% by weight of the layer containing the antioxidant (first layer, second layer, or third layer) is preferably 2% by weight or less.

[0159] <Other Components> The interlayer, the first layer, the second layer, and the third layer may each contain other components other than those described above (thermoplastic resin, plasticizer, heat-shielding substance, metal salt, UV shielding agent, antioxidant) as needed. Examples of these other components include colorants (pigments and dyes, etc.), light-shielding agents, adhesive strength modifiers other than metal salts, light stabilizers, flame retardants, antistatic agents, and moisture-resistant agents. Each of these other components may be used individually or in combination of two or more.

[0160] (Further details of the interlayer for laminated glass) Since the minimum thickness (X μm) of the first layer is 125 μm or more, the average thickness of the first layer is 125 μm or more. The average thickness of the first layer is preferably 130 μm or more, more preferably 140 μm or more, even more preferably 150 μm or more, particularly preferably 160 μm or more, most preferably 170 μm or more, preferably 300 μm or less, more preferably 290 μm or less, more preferably 280 μm or less, more preferably 270 μm or less, more preferably 260 μm or less, more preferably 250 μm or less, more preferably 240 μm or less, more preferably 230 μm or less, more preferably 220 μm or less, more preferably 210 μm or less, more preferably 200 μm or less, more preferably 190 μm or less, even more preferably 180 μm or less, particularly preferably 170 μm or less, and most preferably 160 μm or less. If the average thickness of the first layer is above the lower limit and below the upper limit, the sound insulation in the mid-frequency range can be further improved. In addition, bleed-out can be suppressed more effectively. The average thickness of the first layer may be 125 μm or more, 150 μm or more, 175 μm or more, or 200 μm or more. The average thickness of the first layer may be 200 μm or less, 175 μm or less, or 150 μm or less.

[0161] The minimum thickness of the second layer described above is preferably 300 μm or more, more preferably 350 μm or more, even more preferably 400 μm or more, preferably 700 μm or less, more preferably 600 μm or less, and even more preferably 500 μm or less. When the minimum thickness of the second layer described above is above the lower limit and below the upper limit, the sound insulation performance in the mid-frequency range can be further improved.

[0162] The average thickness of the second layer described above is preferably 300 μm or more, more preferably 350 μm or more, even more preferably 400 μm or more, preferably 700 μm or less, more preferably 600 μm or less, and even more preferably 500 μm or less. If the average thickness of the second layer described above is above the lower limit and below the upper limit, the sound insulation performance in the mid-frequency range can be further improved.

[0163] The minimum thickness of the third layer described above is preferably 300 μm or more, more preferably 350 μm or more, even more preferably 400 μm or more, preferably 700 μm or less, more preferably 600 μm or less, and even more preferably 500 μm or less. When the minimum thickness of the third layer described above is above the lower limit and below the upper limit, the sound insulation performance in the mid-frequency range can be further improved.

[0164] The average thickness of the third layer described above is preferably 300 μm or more, more preferably 350 μm or more, even more preferably 400 μm or more, preferably 700 μm or less, more preferably 600 μm or less, and even more preferably 500 μm or less. If the average thickness of the third layer described above is above the lower limit and below the upper limit, the sound insulation performance in the mid-frequency range can be further improved.

[0165] The ratio of the minimum thickness of the first layer to the minimum thickness of the interlayer (minimum thickness of the first layer / minimum thickness of the interlayer) is preferably 0.10 or more, more preferably 0.13 or more, even more preferably 0.14 or more, particularly preferably 0.15 or more, preferably 0.30 or less, more preferably 0.25 or less, and even more preferably 0.20 or less. When the above ratio (minimum thickness of the first layer / minimum thickness of the interlayer) is above the lower limit and below the upper limit, the sound insulation performance in the mid-frequency range can be further improved. In addition, bleed-out can be suppressed more effectively.

[0166] The ratio of the average thickness of the first layer to the average thickness of the interlayer (average thickness of the first layer / average thickness of the interlayer) is preferably 0.10 or more, more preferably 0.13 or more, even more preferably 0.14 or more, particularly preferably 0.15 or more, preferably 0.30 or less, more preferably 0.25 or less, and even more preferably 0.20 or less. When the above ratio (average thickness of the first layer / average thickness of the interlayer) is above the lower limit and below the upper limit, the sound insulation performance in the mid-frequency range can be further improved. In addition, bleed-out can be suppressed more effectively.

[0167] The ratio of the minimum thickness of the first layer to the minimum thickness of the second layer (minimum thickness of the first layer / minimum thickness of the second layer) is preferably 0.20 or more, more preferably 0.30 or more, even more preferably 0.40 or more, preferably 0.70 or less, more preferably 0.60 or less, and even more preferably 0.50 or less. When the above ratio (minimum thickness of the first layer / minimum thickness of the second layer) is above the lower limit and below the upper limit, the sound insulation performance in the mid-frequency range can be further improved. In addition, bleed-out can be suppressed more effectively.

[0168] The ratio of the average thickness of the first layer to the average thickness of the second layer (average thickness of the first layer / average thickness of the second layer) is preferably 0.20 or more, more preferably 0.30 or more, even more preferably 0.40 or more, preferably 0.70 or less, even more preferably 0.60 or less, and even more preferably 0.50 or less. When the above ratio (average thickness of the first layer / average thickness of the second layer) is above the lower limit and below the upper limit, the sound insulation performance in the mid-frequency range can be further improved. In addition, bleed-out can be suppressed more effectively.

[0169] The ratio of the minimum thickness of the first layer to the minimum thickness of the third layer (minimum thickness of the first layer / minimum thickness of the third layer) is preferably 0.20 or more, more preferably 0.30 or more, even more preferably 0.40 or more, preferably 0.70 or less, more preferably 0.60 or less, and even more preferably 0.50 or less. When the above ratio (minimum thickness of the first layer / minimum thickness of the third layer) is above the lower limit and below the upper limit, the sound insulation performance in the mid-frequency range can be further improved. In addition, bleed-out can be suppressed more effectively.

[0170] The ratio of the average thickness of the first layer to the average thickness of the third layer (average thickness of the first layer / average thickness of the third layer) is preferably 0.20 or more, more preferably 0.30 or more, even more preferably 0.40 or more, preferably 0.70 or less, more preferably 0.60 or less, and even more preferably 0.50 or less. When the above ratio (average thickness of the first layer / average thickness of the third layer) is above the lower limit and below the upper limit, the sound insulation performance in the mid-frequency range can be further improved. In addition, bleed-out can be suppressed more effectively.

[0171] Examples of measuring instruments used to measure the thickness of the above-mentioned interlayer include the contact-type thickness gauge "TOF-4R" (manufactured by Yamabun Electric Co., Ltd.).

[0172] The thickness of the interlayer film described above is measured using the aforementioned measuring instrument, at a film transport speed of 2.15 mm / min to 2.25 mm / min, so as to be the shortest distance from the first end to the second end.

[0173] Furthermore, the "SE-3000" (manufactured by SELMIC Corporation) is an example of a measuring instrument used to measure the thickness of each layer of the interlayer film mentioned above.

[0174] The thickness of each layer of the above interlayer can be measured as follows: Cut the interlayer in the thickness direction at the measurement location using a razor, cutter, etc. After observing the cut surface of the interlayer using the above measuring instrument, measure the thickness of each layer using the calculation software included in the accompanying software.

[0175] Examples of measuring instruments used to measure the thickness of the interlayer after it has been laminated into glass, and the thickness of each layer of the interlayer, include the non-contact multilayer film thickness measuring instrument "OPTIGAUGE" (manufactured by Lumetrix). When using this measuring instrument, the thickness of the interlayer can be measured while the glass is still laminated.

[0176] The second layer is preferably the first surface layer of the interlayer. The third layer is preferably the second surface layer of the interlayer.

[0177] The above-mentioned interlayer may be an interlayer with a uniform thickness, or an interlayer with a varying thickness. The cross-sectional shape of the above-mentioned interlayer may be rectangular, or it may be wedge-shaped.

[0178] The interlayer may be wound to form a roll of interlayer material. The roll may comprise a core and the interlayer material wound around the outer circumference of the core.

[0179] The distance between one end and the other end of the interlayer is preferably 3 m or less, more preferably 2 m or less, particularly preferably 1.5 m or less, preferably 0.5 m or more, more preferably 0.8 m or more, and particularly preferably 1 m or more.

[0180] It is preferable that the glass transition temperature of the first layer and the glass transition temperature of the second layer are different. It is also preferable that the glass transition temperature of the first layer and the glass transition temperature of the third layer are different. The glass transition temperature of the second layer and the glass transition temperature of the third layer may be the same or different.

[0181] The glass transition temperature of the first layer is preferably lower than that of the second layer. In this case, the sound insulation performance in the mid-frequency range can be further improved.

[0182] The glass transition temperature of the first layer is preferably lower than that of the third layer. In this case, the sound insulation performance in the mid-frequency range can be further improved.

[0183] The glass transition temperature of the first layer is preferably -6°C or higher, more preferably -4°C or higher, even more preferably -3°C or higher, preferably 2°C or lower, more preferably 1°C or lower, and even more preferably 0°C or lower. When the glass transition temperature is above the lower limit and below the upper limit, the sound insulation in the mid-frequency range can be further improved.

[0184] The glass transition temperature of the second layer is preferably 19°C or higher, more preferably 22°C or higher, even more preferably 25°C or higher, preferably 35°C or lower, more preferably 32°C or lower, and even more preferably 29°C or lower. When the glass transition temperature is above the lower limit and below the upper limit, the sound insulation in the mid-frequency range can be further improved.

[0185] The glass transition temperature of the third layer is preferably 19°C or higher, more preferably 22°C or higher, even more preferably 25°C or higher, preferably 35°C or lower, more preferably 32°C or lower, and even more preferably 29°C or lower. When the glass transition temperature is above the lower limit and below the upper limit, the sound insulation in the mid-frequency range can be further improved.

[0186] The above glass transition temperature is determined by viscoelasticity measurement. Specifically, the above viscoelasticity measurement is performed as follows.

[0187] A laminate is obtained by sandwiching the above interlayer between two 100 μm thick polyethylene terephthalate films (PET films, for example, Toray Industries' "Lumirror H10"). The obtained laminate is sandwiched between two 2.0 mm thick green glass sheets, placed in a rubber bag, and degassed at a vacuum of 0.08 MPa for 20 minutes. After degassing, the laminate is transferred to an oven in its degassed state and vacuum-pressed at 90°C for 30 minutes to pre-compress the laminate. After pre-compression, the laminate is compressed in an autoclave at 140°C and a pressure of 1.3 MPa for 20 minutes to obtain a test specimen. The test specimen is stored for 4 weeks in an environment with a temperature of 23 ± 2°C and a humidity of 25 ± 5%. After storage, the green glass and PET films are peeled off, and the viscoelasticity is measured using a viscoelasticity measuring device (TA Instruments' viscoelasticity measuring device "ARES-G2" or an equivalent). A parallel plate with a diameter of 8 mm is used as a jig, and measurements are taken under the conditions of shear mode, a cooling rate of 3 °C / min from 100 °C to -20 °C, and a frequency of 1 Hz and a strain of 1%. In the obtained measurement results, the peak temperature of the loss tangent is defined as the glass transition temperature Tg (°C). Although the interlayer has a structure of three or more layers, the above test specimen is prepared in an integrated state without separation, and measurements are taken, and the glass transition temperature etc. derived from each layer are read from the measurement results. In the case of laminated glass, after cooling the laminated glass with liquid nitrogen or the like, the laminated glass member and the interlayer are separated, and the above test specimen is prepared using the separated interlayer by the method described above. The above viscoelasticity measurement is performed using this test specimen.

[0188] The method for manufacturing the above-mentioned interlayer film is not particularly limited. Examples of methods for manufacturing the interlayer film include a method in which each layer is formed using each resin composition for forming each layer, and then the resulting layers are laminated, and a method in which each layer is laminated by co-extruding each resin composition for forming each layer using an extruder. A manufacturing method using extrusion molding is preferred because it is suitable for continuous production.

[0189] It is preferable that the second layer and the third layer contain the same thermoplastic resin, as this improves the efficiency of interlayer production. It is more preferable that the second layer and the third layer contain the same thermoplastic resin and the same plasticizer, as this improves the efficiency of interlayer production. It is preferable that the second layer and the third layer contain the same polyvinyl acetal resin, as this improves the efficiency of interlayer production. It is more preferable that the second layer and the third layer contain the same polyvinyl acetal resin and the same plasticizer, as this improves the efficiency of interlayer production. It is even more preferable that the second layer and the third layer are formed from the same resin composition, as this improves the efficiency of interlayer production. It is even more preferable that the second layer and the third layer have the same composition, as this improves the efficiency of interlayer production.

[0190] The interlayer film described above preferably has an uneven surface on at least one of its two surfaces. It is more preferable that the interlayer film has an uneven surface on both surfaces. The method for forming the uneven surface is not particularly limited and includes, for example, lip embossing, embossing roll, calendering roll, and shape extrusion. Embossing roll is preferred because it can form a large number of uneven patterns that are quantitatively consistent.

[0191] (Laminated Glass) The laminated glass according to the present invention comprises a first laminated glass member, a second laminated glass member, and the above-described interlayer for laminated glass. In the laminated glass according to the present invention, the above-described interlayer for laminated glass is arranged between the first laminated glass member and the second laminated glass member.

[0192] Furthermore, the present invention also provides the following laminated glass. The laminated glass according to the present invention comprises a first laminated glass member, a second laminated glass member, and an interlayer for laminated glass having a structure of three or more layers. In the laminated glass according to the present invention, the interlayer is disposed between the first laminated glass member and the second laminated glass member. In the laminated glass according to the present invention, the interlayer comprises a first layer, a second layer, and a third layer, wherein the second layer is disposed on the first surface side of the first layer, and the third layer is disposed on the second surface side of the first layer opposite to the first surface. In the laminated glass according to the present invention, the interlayer contains a thermoplastic resin and a plasticizer. In the present invention, the minimum thickness of the first layer is X μm, the content of the plasticizer in the interlayer relative to 100 parts by weight of the thermoplastic resin in the interlayer is Y parts by weight, and the primary resonant frequency of the laminated glass is Z Hz. The laminated glass according to the present invention comprises at least one of the following configurations A, B, and C.

[0193] Configuration A: 125 ≤ X, and 40 ≤ Y ≤ 44

[0194] Configuration B: 125 ≤ X ≤ 250, and -0.0076X + 42.054 ≤ Y ≤ -0.0096X + 45.330

[0195] Configuration C: 125 ≤ X ≤ 250, and 125 ≤ Z ≤ 140

[0196] The laminated glass according to the present invention has the above configuration, which makes it possible to improve sound insulation in the medium frequency range (2500 Hz to 4000 Hz).

[0197] The laminated glass may comprise at least configuration A, at least configuration B, and at least configuration C. The laminated glass may comprise at least one of configuration A and configuration B, at least one of configuration A and configuration C, and at least one of configuration B and configuration C. The laminated glass may comprise at least configuration A and configuration B, at least configuration A and configuration C, at least configuration B and configuration C, and configuration A, configuration B, and configuration C. The laminated glass may comprise at least two of configuration A, configuration B, and configuration C.

[0198] From the viewpoint of improving sound insulation in the mid-frequency range, it is preferable that the laminated glass comprises at least the above configuration C, and more preferably that it comprises at least the above configuration B and the above configuration C.

[0199] Furthermore, the preferred ranges of configurations A, B, and C in the laminated glass described above are the same as the preferred ranges of configurations A, B, and C in the interlayer described above. Also, the preferred configurations of the interlayer, the first layer, the second layer, and the third layer in the laminated glass described above are the same as the preferred configurations of the interlayer, the first layer, the second layer, and the third layer described above. In addition, the primary resonance frequency of the laminated glass can be measured in the same manner as the method for measuring the primary resonance frequency of the laminated glass G described above.

[0200] Figure 2 is a schematic cross-sectional view showing an example of laminated glass using the interlayer film for laminated glass shown in Figure 1.

[0201] Figure 2 is a cross-sectional view of the laminated glass 31 along the thickness direction. The laminated glass 31 comprises a first laminated glass member 21, a second laminated glass member 22, and an interlayer 11. The interlayer 11 is positioned between the first laminated glass member 21 and the second laminated glass member 22. The first laminated glass member 21 is positioned on the first surface side of the interlayer 11 and is laminated with it. The second laminated glass member 22 is positioned on the second surface side of the interlayer 11, opposite to the first surface, and is laminated with it.

[0202] Thus, the laminated glass comprises a first laminated glass member, a second laminated glass member, and an interlayer. In the laminated glass, the interlayer is positioned between the first laminated glass member and the second laminated glass member.

[0203] The first laminated glass member described above is preferably a first glass plate. The second laminated glass member described above is preferably a second glass plate.

[0204] Examples of the first and second laminated glass members mentioned above include glass plates and PET (polyethylene terephthalate) films. The laminated glass includes not only laminated glass in which an interlayer is sandwiched between two glass plates, but also laminated glass in which an interlayer is sandwiched between a glass plate and a PET film or the like. The laminated glass is a laminate comprising glass plates, and it is preferable that at least one glass plate is used. It is preferable that the first laminated glass member and the second laminated glass member are each glass plates or PET films, and that the laminated glass comprises a glass plate as at least one of the first laminated glass member and the second laminated glass member. It is particularly preferable that both the first and second laminated glass members are glass plates.

[0205] Examples of the above-mentioned glass plates include inorganic glass and organic glass. Examples of the above-mentioned inorganic glass include float glass, heat-absorbing glass, heat-reflective glass, polished glass, patterned glass, wired glass, and green glass. Examples of the above-mentioned organic glass include synthetic resin glass that can be used as an alternative to inorganic glass. Examples of the above-mentioned organic glass include polycarbonate sheets and poly(meth)acrylic resin sheets. Examples of the above-mentioned poly(meth)acrylic resin sheets include polymethyl (meth)acrylate sheets.

[0206] The thickness of the first laminated glass member and the second laminated glass member described above is preferably 1 mm or more, preferably 5 mm or less, and more preferably 3 mm or less. Furthermore, if the laminated glass member is a glass plate, the thickness of the glass plate is preferably 0.5 mm or more, more preferably 0.7 mm or more, preferably 5 mm or less, and more preferably 3 mm or less. If the laminated glass member is a PET film, the thickness of the PET film is preferably 0.03 mm or more, and more preferably 0.5 mm or less.

[0207] The method for manufacturing the laminated glass described above is not particularly limited. The laminated glass can be manufactured, for example, as follows: First, an interlayer is sandwiched between the first laminated glass member and the second laminated glass member to obtain a laminate. Next, the air remaining between the first laminated glass member, the second laminated glass member and the interlayer is removed, for example, by passing the obtained laminate through a pressing roll or by placing it in a rubber bag and applying reduced pressure and suction. After that, the laminate is pre-bonded at approximately 70°C to 110°C to obtain a pre-compressed laminate. Next, the pre-compressed laminate is placed in an autoclave or pressed to compress it at approximately 120°C to 150°C and a pressure of 1 MPa to 1.5 MPa. In this way, laminated glass can be obtained.

[0208] The above-mentioned interlayer and laminated glass can be used in automobiles, railway vehicles, aircraft, ships, and buildings, etc. The above-mentioned interlayer and laminated glass can also be used for purposes other than those listed above. The above-mentioned interlayer and laminated glass are preferably interlayers and laminated glass for vehicles or buildings, and more preferably interlayers and laminated glass for vehicles. The above-mentioned interlayer and laminated glass can be used in automobile windshields, automobile side windows, automobile rear windows, automobile roof windows, or automobile taillight glass, etc., and are particularly suitable for use in automobile windshields. The above-mentioned interlayer and laminated glass are suitably used in automobiles. The above-mentioned interlayer is suitably used to obtain automobile laminated glass. Specific embodiments of the use of the above-mentioned interlayer include the following: Use of the above-mentioned interlayer in laminated glass. Use of the above-mentioned interlayer in laminated glass for vehicles or buildings. Use of the above-mentioned interlayer in laminated glass for vehicles. Use of the above-mentioned interlayer in laminated glass for automobiles. Use of the above-mentioned interlayer in automobile windshields, automobile side windows, automobile rear windows, automobile roof windows, or automobile taillight glass. Use of the above-mentioned interlayer in the windshield of an automobile.

[0209] The present invention will be specifically described below with reference to examples and comparative examples. The present invention is not limited to the following examples.

[0210] In the polyvinyl acetal resin used, n-butyraldehyde with 4 carbon atoms was used for acetalization. The degree of acetalization (butyralization), degree of acetylation, and hydroxyl group content of the polyvinyl acetal resin were measured using a Bruker Ascend 400 nuclear magnetic resonance spectrometer and JEOL Delta analysis software, according to the method described above. Since the ends of peaks B and C, C and D, and D and E overlapped, the minimum value between each peak was used as the delimiter during integration.

[0211] The following materials were prepared.

[0212] (Thermoplastic resins) PVB1: Polyvinyl acetal resin (polyvinyl butyral resin), average degree of polymerization 3000, hydroxyl group content 20.4 mol%, degree of acetylation 13.0 mol%, degree of acetalization (degree of butyralization) 66.6 mol% PVB2: Polyvinyl acetal resin (polyvinyl butyral resin), average degree of polymerization 1700, hydroxyl group content 29.2 mol%, degree of acetylation 1.3 mol%, degree of acetalization (degree of butyralization) 69.5 mol%

[0213] (Plasticizer) 3GO: Triethylene glycol di-2-ethylhexanoate

[0214] (Metal salt) Mg mixture (50:50 (by weight ratio) mixture of magnesium 2-ethylbutyrate and magnesium acetate)

[0215] (UV shielding agent) Tinuvin 326: 2-(2'-hydroxy-3'-t-butyl-5-methylphenyl)-5-chlorobenzotriazole (BASF's "Tinuvin 326")

[0216] (Antioxidant) BHT: 2,6-di-t-butyl-p-cresol

[0217] (Example 1) Preparation of resin composition for forming the first layer: The following components were blended and thoroughly kneaded with a mixing roll to obtain a resin composition for forming the first layer.

[0218] PVB1: 100 parts by weight 3GO: 73.7 parts by weight Mg mixture: an amount that results in a magnesium content of 70 ppm in the resulting first layer Tinuvin 326: an amount that results in a 0.2% by weight in the resulting first layer BHT: an amount that results in a 0.2% by weight in the resulting first layer

[0219] Preparation of resin compositions for forming the second and third layers: The following components were blended and thoroughly kneaded with a mixing roll to obtain resin compositions for forming the second and third layers.

[0220] PVB2: 100 parts by weight 3GO: 37.6 parts by weight Mg mixture: an amount that results in a magnesium content of 70 ppm in the resulting second and third layers Tinuvin 326: an amount that results in a 0.2% by weight in the resulting second and third layers BHT: an amount that results in a 0.2% by weight in the resulting second and third layers

[0221] Interlayer preparation: An interlayer (thickness 852 μm) having a laminated structure of second layer (thickness 351 μm) / first layer (thickness 150 μm) / third layer (thickness 351 μm) was prepared by co-extruding a resin composition for forming the first layer and resin compositions for forming the second and third layers using a co-extruder. Since the obtained interlayer and each layer have a uniform thickness, the minimum thickness of the interlayer is the same as the average thickness of the interlayer, the minimum thickness of the first layer is the same as the average thickness of the first layer, the minimum thickness of the second layer is the same as the average thickness of the second layer, and the minimum thickness of the third layer is the same as the average thickness of the third layer.

[0222] Preparation of laminated glass: A laminate was obtained by sandwiching an interlayer between two sheets of clear glass measuring 25 mm in width, 300 mm in length, and 2.1 mm in thickness, in accordance with JIS R3202:1996. The obtained laminate was placed in a rubber bag, degassed at a vacuum of 2.6 kPa for 20 minutes, then transferred to an oven while still degassed, and vacuum-pressed at 90°C for 30 minutes to pre-compress the laminate. The pre-compressed laminate was then compressed in an autoclave at 135°C and a pressure of 1.2 MPa for 20 minutes to obtain laminated glass. The obtained laminated glass corresponds to the laminated glass G described above.

[0223] (Examples 2-13 and Comparative Examples 1-9) Interlayers and laminated glass were obtained in the same manner as in Example 1, except that the plasticizer content and the thickness of each layer were changed as shown in the table below. Since the obtained interlayers and each layer have a uniform thickness, the minimum thickness of the interlayer is the same as the average thickness of the interlayer, the minimum thickness of the first layer is the same as the average thickness of the first layer, the minimum thickness of the second layer is the same as the average thickness of the second layer, and the minimum thickness of the third layer is the same as the average thickness of the third layer.

[0224] (Evaluation) (1) Primary Resonance Frequency of Laminated Glass The laminated glass (laminated glass G) was stored for 4 weeks in an environment with a temperature of 23±2°C and a humidity of 25±5%. After storage, laminated glass G was excited in a constant temperature chamber at 20°C using a vibration generator for damping tests (Spectris "Pertable Vibration Exciter Type 4809"). The obtained vibration characteristics were amplified using a mechanical impedance measuring device (Spectris "75 VA Power Amplifier Type 2718"), and the primary resonance frequency was determined by FFT analysis of the vibration spectrum. Spectris "PULSE LabShop" was used as the analysis software.

[0225] (2) A laminate was obtained by sandwiching the obtained interlayer between two polyethylene terephthalate films (PET films, "Lumirror H10" manufactured by Toray Industries, Inc.) with a bleed-out thickness of 100 μm. The obtained laminate was sandwiched between two 2.0 mm thick green glass sheets, placed in a rubber bag, and degassed at a vacuum of 0.08 MPa for 20 minutes. After degassing, the laminate was moved to an oven in its degassed state and vacuum-pressed at 90°C for 30 minutes to pre-compress the laminate. After pre-compression, the laminate was compressed in an autoclave at 140°C and a pressure of 1.3 MPa for 20 minutes, then cut into 150 mm x 150 mm squares, and the polyethylene terephthalate film was peeled off to obtain test specimens. On the obtained test specimens, lines were drawn in a grid pattern (parallel crosses) using a red oil-based pen (Magic Ink, Teranishi Chemical Industry Co., Ltd. "ML-T2 Red") (line length: 110 mm, line width: 5.0 mm, line intersections: 30 mm from both ends of the line). The test specimens were fixed so that the surface with the lines drawn was perpendicular to the ground, and left to stand for 3 days in an environment with a temperature of 10 ± 2°C. After standing, the length of the ink trail that dripped from the red lines on the surface of the test specimens in the direction of gravity was measured.

[0226] [Criteria for determining bleed-out] ○: Ink stain length is less than 1 cm △: Ink stain length is 1 cm or more but less than 3 cm ×: Ink stain length is 3 cm or more

[0227] (3) Sound Insulation in the Mid-Frequency Range The sound insulation in the mid-frequency range was evaluated by measuring the sound transmission loss in accordance with JIS A1416:2000. Sound transmission loss is a numerical value that represents the sound insulation performance of a material and represents the amount of reduction in the energy of transmitted sound relative to incident sound. The larger the value of sound transmission loss, the higher the sound insulation performance. The values ​​in the table below are the sound transmission losses at center frequencies of 2500 Hz, 3150 Hz, and 4000 Hz in 1 / 3 octave band analysis, as well as their average values.

[0228] The composition and results of the interlayer are shown in Tables 1 to 5 below.

[0229]

[0230]

[0231]

[0232]

[0233]

[0234] 1...First layer 1a...First surface 1b...Second surface 2...Second layer 3...Third layer 11...Interlayer 21...First laminated glass member 22...Second laminated glass member 31...Laminated glass

Claims

1. An interlayer for laminated glass having a structure of three or more layers, comprising a first layer, a second layer, and a third layer, wherein the second layer is disposed on the first surface side of the first layer, and the third layer is disposed on the second surface side of the first layer opposite to the first surface, the interlayer contains a thermoplastic resin and a plasticizer, the minimum thickness of the first layer is X μm, the content of the plasticizer in the interlayer relative to 100 parts by weight of the thermoplastic resin in the interlayer is Y parts by weight, and when the primary resonance frequency of laminated glass G obtained by distributing the interlayer between two clear glass sheets with a thickness of 2.1 mm is Z Hz, the interlayer comprises at least one of the following configurations A, B, and C. Configuration A: 125 ≤ X, and 40 ≤ Y ≤ 44 Configuration B: 125 ≤ X ≤ 250, and -0.0076X + 42.054 ≤ Y ≤ -0.0096X + 45.330 Configuration C: 125 ≤ X ≤ 250, and 125 ≤ Z ≤ 140 2. The interlayer for laminated glass according to claim 1, comprising at least the above-mentioned configuration A.

3. The interlayer for laminated glass according to claim 1 or 2, comprising at least the above-mentioned configuration B.

4. The interlayer for laminated glass according to any one of claims 1 to 3, comprising at least the above-mentioned configuration C.

5. The interlayer for laminated glass according to any one of claims 1 to 4, comprising at least the above-mentioned configuration B and configuration C.

6. The interlayer for laminated glass according to any one of claims 1 to 5, wherein the first layer comprises a thermoplastic resin and a plasticizer.

7. The interfilm for laminated glass according to claim 6, wherein the thermoplastic resin in the first layer is a polyvinyl acetal resin.

8. The interlayer for laminated glass according to any one of claims 1 to 7, wherein the second layer comprises a thermoplastic resin and a plasticizer, and the third layer comprises a thermoplastic resin and a plasticizer.

9. The interlayer film for laminated glass according to claim 8, wherein the content of the plasticizer in the first layer relative to 100 parts by weight of the thermoplastic resin in the first layer is greater than the content of the plasticizer in the second layer relative to 100 parts by weight of the thermoplastic resin in the second 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 is greater than the content of the plasticizer in the third layer relative to 100 parts by weight of the thermoplastic resin in the third layer.

10. The interlayer for laminated glass according to any one of claims 1 to 9, wherein the ratio of the minimum thickness of the first layer to the minimum thickness of the interlayer is 0.14 or more and 0.25 or less.

11. An interlayer for laminated glass according to any one of claims 1 to 10, wherein the glass transition temperature of the first layer is lower than the glass transition temperature of the second layer, and the glass transition temperature of the first layer is lower than the glass transition temperature of the third layer.

12. Laminated glass comprising a first laminated glass member, a second laminated glass member, and an interlayer for laminated glass according to any one of claims 1 to 11, wherein the interlayer is disposed between the first laminated glass member and the second laminated glass member.

13. A laminated glass comprising a first laminated glass member, a second laminated glass member, and an interlayer for laminated glass having a structure of three or more layers, wherein the interlayer is disposed between the first laminated glass member and the second laminated glass member, the interlayer comprises a first layer, a second layer, and a third layer, the second layer is disposed on the first surface side of the first layer, the third layer is disposed on the second surface side of the first layer opposite to the first surface, the interlayer contains a thermoplastic resin and a plasticizer, the minimum thickness of the first layer is X μm, the content of the plasticizer in the interlayer relative to 100 parts by weight of the thermoplastic resin in the interlayer is Y parts by weight, and the primary resonant frequency of the laminated glass is Z Hz, wherein the laminated glass comprises at least one of the following configurations A, B, and C. Configuration A: 125 ≤ X, and 40 ≤ Y ≤ 44 Configuration B: 125 ≤ X ≤ 250, and -0.0076X + 42.054 ≤ Y ≤ -0.0096X + 45.330 Configuration C: 125 ≤ X ≤ 250, and 125 ≤ Z ≤ 140

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