INTERMEDIATE FILM FOR LAMINATED GLASS, AND LAMINATED GLASS

专利摘要:
INTERMEDIATE FILM FOR LAMINATED GLASS, AND LAMINATED GLASS. The invention relates to an intermediate film for laminated glass which makes a portion of the edge of the laminated glass less susceptible to formation of an opening and is able to suppress the increase in the YI value at the edge portion of the laminated glass. An intermediate film for laminated glass in accordance with the present invention is provided with: a first layer which contains a polyvinyl acetal resin and a plasticizer; and a second layer which is arranged on a first surface of the first layer and contains a polyvinyl acetal resin and a plasticizer. The first layer additionally contains a hindered amine light stabilizer in which an alkyl group or an alkoxy group is attached to the nitrogen atom of a piperidine structure. The second layer has a glass transition temperature of 32°C or more.
公开号:BR112016021517B1
申请号:R112016021517-6
申请日:2015-03-27
公开日:2021-08-03
发明作者:Tatsuya Iwamoto；Shougo Yoshida
申请人:Sekisui Chemical Co., Ltd；
IPC主号:

专利说明:

TECHNICAL FIELD
[0001] The present invention relates to an interlayer film for laminated glass used for laminated glass. Furthermore, the present invention relates to laminated glass prepared with the interlayer film for laminated glass. BACKGROUND OF THE INVENTION
[0002] Since laminated glass only generates a small amount of scattered glass fragments even when subjected to an external impact and broken, laminated glass is excellent in safety. In this way, laminated glass is widely used for automobiles, railway vehicles, airplanes, ships, buildings, and the like. Laminated glass is produced by sandwiching an interlayer film for laminated glass between a pair of glass plates.
[0003] As an example of the interlayer film for laminated glass, Patent Document 1 below discloses an interlayer film which has a low tendency to yellow, has a high transmittance for UV-A rays and visible light, and it has a low transmittance for UV-B rays. This interlayer film includes a polyvinyl acetal, a plasticizer and an oxanilide-based compound as a UV absorber. Furthermore, in Patent Document 1, a technique for allowing a non-aromatic light stabilizer of the HAS/HALS/NOR-HALS type to be included in the interlayer film is described.
[0004] Patent Document 2 below discloses an interlayer film which is high in ultraviolet ray blocking characteristics and manages to maintain an optical quality for a long period of time. This interlayer film includes a polymer layer. The polymer layer includes a tungsten oxide reagent and at least one type between a molecule having a benzotriazole group and a polyvalent metal salt.
[0005] Patent Document 3 below discloses an interlayer film with which the sound insulation properties in a high frequency area of laminated glass can be enhanced over a wide temperature range. This interlayer film is provided with a first layer which contains a polyvinyl acetal resin and a plasticizer, a second layer which is arranged on a first surface of the first layer and contains a polyvinyl acetal resin and a plasticizer, and a third layer which is arranged on a second surface opposite the first surface of the first layer and contains a polyvinyl acetal resin and a plasticizer. In this interlayer film, the hydroxyl group content of the polyvinyl acetal resin contained in the first layer is lower than the content of each hydroxyl group of the polyvinyl acetal resins contained in the second and third layers, and the ratio of the thickness of the first layer and the total thickness of the second layer and the third layer is less than or equal to 0.14. Furthermore, in Patent Document 3, a technique is described which can obtain laminated glass in which foam generation and bubble growth can be suppressed. Related Art Document Patent Document Patent Document 1: U.S. 2012/0052310 A1 Patent Document 2: U.S. 2009/0035583 A1 Patent Document 3: WO 2012/043816 A1 BRIEF DESCRIPTION OF THE INVENTION PROBLEMS TO BE SOLVED BY THE INVENTION
[0006] In the end part of the laminated glass sheet prepared with a conventional interlayer film, an opening is sometimes generated. In particular, this opening is easily generated when light, heat and the like are applied to the laminated glass sheet. This opening is a recess portion formed by omitting the film between layers at the end portion of the laminated glass sheet. This opening is different from a foam product generated due to foam formation as described in Patent Document 3.
[0007] When an opening is generated in the end part of the laminated glass sheet, the appearance of the laminated glass sheet is deteriorated and the adhesion force between the film between layers and a glass plate or the like is reduced.
[0008] Furthermore, when a laminated glass sheet is prepared with a conventional interlayer film, the yellow index (YI) value measured at the end portion of the laminated glass sheet is sometimes increased.
[0009] An object of the present invention is to provide an interlayer film for laminated glass by making an opening difficult to be generated in an end portion of the laminated glass sheet and by allowing an increase in the YI value measured at the end part of the laminated glass sheet is suppressed. MEANS TO SOLVE PROBLEMS
[0010] According to a broad aspect of the present invention, there is provided an interlayer film for laminated glass that includes a first layer that contains a polyvinyl acetal resin and a plasticizer and a second layer that is arranged on one side of the first surface of the first layer and contains a polyvinyl acetal resin and a plasticizer, wherein the first layer also contains a hindered amine light stabilizer that has an alkyl group attached to the nitrogen atom of a piperidine structure or an alkoxy group attached to the nitrogen atom of a piperidine structure, where the second layer has a glass transition temperature higher than or equal to 32°C.
[0011] In a specific aspect of the interlayer film for laminated glass according to the present invention, at least a first metal atom selected from the group consisting of an alkaline earth metal, zinc and aluminum is included in the interlayer film, a metal alkali is not included or else is included in the interlayer film, and the content of the first metal atom in the interlayer film is less than or equal to 150 ppm.
[0012] In a specific aspect of the interlayer film for laminated glass according to the present invention, the content of plasticizer contained in the first layer in relation to 100 parts by weight of the polyvinyl acetal resin contained in the first layer is greater than the content of plasticizer contained in the second layer with respect to 100 parts by weight of the polyvinyl acetal resin contained in the second layer.
[0013] In a specific aspect of the interlayer film for laminated glass according to the present invention, the polyvinyl acetal resin contained in the first layer is obtained by means of the acetalization of a polyvinyl alcohol with an average degree of polymerization greater than or equal to 1,500.
[0014] In a specific aspect of the interlayer film for laminated glass according to the present invention, the degree of acetylation of the polyvinyl acetal resin contained in the first layer is greater than or equal to 0.1% in mol and less than than or equal to 25% by mol, and the hydroxyl group content of the polyvinyl acetal resin contained in the first layer is greater than or equal to 20% by mol and less than 30% by mol.
[0015] In a specific aspect of the interlayer film for laminated glass according to the present invention, the glass transition temperature of the first layer is lower than or equal to 20°C.
[0016] In a specific aspect of the interlayer film for laminated glass according to the present invention, the first layer contains an oxidation inhibitor that has a molecular weight greater than or equal to 250 and includes a phenol skeleton.
[0017] In a specific aspect of the interlayer film for laminated glass according to the present invention, the molecular weight of the hindered amine light stabilizer is less than or equal to 1,000.
[0018] In a specific aspect of the interlayer film for laminated glass according to the present invention, the interlayer film for laminated glass also includes a third layer which is arranged on a side of the second surface opposite the first surface of the first layer and contains a polyvinyl acetal resin and a plasticizer.
[0019] In a specific aspect of the interlayer film for laminated glass according to the present invention, the glass transition temperature of the third layer is higher than or equal to 32°C.
[0020] In a specific aspect of the interlayer film for laminated glass according to the present invention, the interlayer film for laminated glass is used to obtain the laminated glass of an automobile.
[0021] According to a broad aspect of the present invention, there is provided a laminated glass which includes a first laminated glass member, a second laminated glass member and an interlayer film for the laminated glass described above, wherein the interlayer film layers for laminated glass is arranged between the first laminated glass member and the second laminated glass member. EFFECT OF THE INVENTION
[0022] Since the interlayer film for laminated glass according to the present invention includes a first layer that contains a polyvinyl acetal resin and a plasticizer and a second layer that is arranged on one side of the first surface of the first layer and contains a polyvinyl acetal resin and a plasticizer, in addition, the first layer also contains an amine light stabilizer that allows an alkyl group attached to the nitrogen atom of a piperidine structure or an alkoxy group attached to the nitrogen atom of a piperidine structure, and the second layer has a glass transition temperature higher than or equal to 32°C, an opening is difficult to be generated in an end portion of the laminated glass sheet prepared with the interlayer film for laminated glass according to the present invention, and an increase in the YI value measured at the end portion of the laminated glass sheet can be suppressed.
[0023] With regard to the interlayer film for laminated glass according to the present invention, since the first layer contains a hindered amine light stabilizer which has an alkyl group attached to the nitrogen atom of a piperidine structure or an alkoxy group attached to the nitrogen atom of a piperidine structure, an opening becomes difficult to be generated in an end portion of the laminated glass sheet and an increase in the YI value measured in the end portion of the laminated glass sheet may be deleted. Furthermore, with regard to the interlayer film for laminated glass according to the present invention, since the glass transition temperature of the second layer is higher than or equal to 32°C, an opening becomes difficult to be generated at an end part of the laminated glass sheet and an increase in the YI value measured at the end part of the laminated glass sheet can be suppressed. BRIEF DESCRIPTION OF THE DRAWINGS
[0024] Figure 1 is a partially detached sectional view schematically showing an interlayer film for laminated glass according to an embodiment of the present invention.
[0025] Figure 2 is a partially detached sectional view that schematically shows an example of laminated glass prepared with the interlayer film for laminated glass shown in Figure 1. WAY TO CARRY OUT THE INVENTION
[0026] In the following, the present invention will be elucidated by describing specific embodiments and examples of the present invention with reference to the drawings.
[0027] Figure 1 shows an interlayer film for laminated glass according to an embodiment of the present invention schematically represented as a partially detached sectional view.
[0028] An interlayer film 1 shown in Figure 1 is an interlayer film having multiple layers that has a structure of two or more layers. Interlayer film 1 is used to obtain laminated glass. The interlayer film 1 has a structure of two or more layers. The interlayer film 1 is an interlayer film for laminated glass. The interlayer film 1 is provided with a first layer 2, a second layer 3 arranged on one side of the first surface 2a of the first layer 2, and a third layer 4 arranged on a side of the second surface 2b opposite the first surface 2a of the first layer 2. The second layer 3 is arranged on the first surface 2a of the first layer 2. The third layer 4 is arranged on the second surface 2b of the first layer 2. The first layer 2 is an intermediate layer. For example, second layer 3 and third layer 4 are protective layers and are surface layers in the present embodiment. The first layer 2 is arranged between the second layer 3 and the third layer 4 to be sandwiched. Therefore, the interlayer film 1 has a multilayer structure in which the second layer 3, the first layer 2 and the third layer 4 are arranged in that order.
[0029] It is preferable that a surface 3a on an opposite side to the side of the first layer 2 of the second layer 3 is a surface on which a laminated glass member is arranged. It is preferable that a surface 4a on a side opposite the first side of layer 2 of the third layer 4 is a surface on which a laminated glass member is arranged.
[0030] In this regard, other layers can be arranged between the first layer 2 and the second layer 3 and between the first layer 2 and the third layer 4, respectively. It is preferred that each of the second layer 3 and the third layer 4 be arranged directly over the first layer 2. Examples of another layer include a layer containing a thermoplastic resin such as a polyvinyl acetal resin, and a layer which contains polyethylene terephthalate, and the like.
[0031] Each of the first layer 2 and the second layer 3 contains a polyvinyl acetal resin and a plasticizer. The first layer 2 contains a hindered amine light stabilizer. The hindered amine light stabilizer has a piperidine structure. The hindered amine light stabilizer contained in the first layer 2 is a hindered amine light stabilizer that permits an alkyl group bonded to the nitrogen atom of a piperidine structure or an alkoxy group bonded to the nitrogen atom of a piperidine structure. The glass transition temperature of the second layer 3 is higher than or equal to 32°C.
[0032] Since the interlayer film 1 is provided with the configuration described above, an opening becomes difficult to be generated in an end part of the laminated glass sheet prepared with the interlayer film 1, and an increase in the value of YI measured at the end part of the laminated glass sheet can be suppressed. With regard to the interlayer film 1, even when a laminated glass sheet prepared with the interlayer film 1 is irradiated with light for a long period of time and the laminated glass sheet can stay at a high temperature for a long time. period of time, it is possible to make an opening difficult to be generated in an end part of the laminated glass sheet. Furthermore, even when a laminated glass sheet prepared with the interlayer films 1 can stay at a high temperature for a long period of time, an increase in the YI value can be suppressed. In this regard, the opening is a recess portion formed by omitting the interlayer film into it at the end portion of the laminated glass sheet. For example, the interlayer film is shrunk inward, and the recess portion is formed.
[0033] X) With regard to the interlayer film 1, since the first layer 2 contains a hindered amine light stabilizer of an alkyl group attached to the nitrogen atom of a piperidine structure or of an attached alkoxy group to the nitrogen atom of a piperidine structure, an opening is difficult to be generated at an end portion of the laminated glass sheet, and an increase in the YI value measured at the end portion of the laminated glass sheet can be suppressed. Furthermore, Y) with respect to the film between layers 1, since the glass transition temperature of the second layer 3 is higher than or equal to 32°C, an opening is difficult to be generated in a separate part. of the laminated glass sheet and allows an increase in the YI value measured at the end portion of the laminated glass sheet to be suppressed. By virtue of the aforementioned configuration of X) and the aforementioned configuration of Y), an effect of making an opening difficult to be generated in an end part of the laminated glass sheet and an effect of allowing an increase in the value of YI measured at the end part of the laminated glass sheet is suppressed are exerted synergistically. It was first verified by the authors of the present invention that such a combination of these effects is obtained by virtue of the aforementioned configuration of X) and the aforementioned configuration of Y) and that these effects are synergistically exerted by virtue of the aforementioned configuration of X) and the aforementioned configuration of Y).
[0034] With regard to the film between layers 1, each of the second layer 3 and the third layer 4 is arranged on both sides of the first layer 2, respectively. The second layer only needs to be arranged on the side of the first surface of the first layer. The second layer is arranged on the first surface side of the first layer, and the third layer need not be arranged on the second surface side of the first layer. In this context, the second layer is arranged on the side of the first surface of the first layer, and it is preferable that the third layer is arranged on the second side of the surface of the first layer. By allowing the third layer to be arranged on the second surface side of the first layer, the interlayer film handling properties and the penetration resistance of the laminated glass are further enhanced. Furthermore, an opening becomes even more difficult to be generated in an end part of the laminated glass sheet, and an increase in the YI value measured in the end part of the laminated glass sheet can also be suppressed. In addition, on the surfaces of both sides of the interlayer film, the adhering ability to a laminated glass member and the like can be adjusted. In this regard, in the case where the third layer is absent, the adhering ability of an outer surface of the second layer of interlayer film to a laminated glass member can be adjusted.
[0035] Furthermore, from the point of view of further enhancing the penetration resistance of the laminated glass prepared with the interlayer film, it is preferable that the third layer contains a polyvinyl acetal resin, it is preferable that the third layer contains an agent plasticizer and it is preferred that the third layer contains a polyvinyl acetal resin and a plasticizer. From the viewpoints of effectively rendering an opening difficult to be generated in an end portion of the laminated glass sheet and of effectively suppressing an increase in the value of YI measured at the end portion of the laminated glass sheet, it is preferable that the temperature of third layer glass transition is higher than or equal to 32°C and therefore it is preferable that the second layer and third layer glass transition temperatures are higher than or equal to 32°C. It is preferable that the interlayer film is provided with the second layer as a surface layer of the interlayer film. It is preferable that the interlayer film is provided with the third layer as a surface layer of the interlayer film.
[0036] From the viewpoints of effectively rendering an opening difficult to be generated in an end portion of the laminated glass sheet and of effectively suppressing an increase in the value of YI measured at the end portion of the laminated glass sheet, the temperature of second layer glass transition is preferably higher than or equal to 33°C and more preferably higher than or equal to 35°C. From the viewpoints of effectively rendering an opening difficult to be generated in an end portion of the laminated glass sheet and of effectively suppressing an increase in the YI value measured at the end portion of the laminated glass sheet, the glass transition temperature of the third layer is preferably higher than or equal to 32°C, more preferably higher than or equal to 33°C and even more preferably higher than or equal to 35°C. The upper limit of the glass transition temperature of each of the second layer and the third layer is not particularly limited. From the standpoint of further enhancing the sound insulation properties of the interlayer film, the glass transition temperature of each of the second layer and the third layer may be lower than or equal to 60°C.
[0037] Next, the details of the first layer, the second layer and the third layer that constitute the interlayer film for laminated glass according to the present invention will be described, and the details of each ingredient contained in the first layer, in the second layer and the third layer.(Polyvinyl acetal resin)
[0038] The first layer contains a polyvinyl acetal resin (hereafter sometimes described as a polyvinyl acetal resin (1)). The second layer contains a polyvinyl acetal resin (hereafter sometimes described as a polyvinyl acetal resin (2)). It is preferable that the third layer contains a polyvinyl acetal resin (hereinafter sometimes described as a polyvinyl acetal resin (3)). The polyvinyl acetal resin (1), the polyvinyl acetal resin (2) and the polyvinyl acetal resin (3) can be the same or different from each other. One type of each of polyvinyl acetal resin (1), polyvinyl acetal resin (2) and polyvinyl acetal resin (3) can be used alone, and two or more types thereof can be used in combination.
[0039] For example, polyvinyl acetal resin can be produced by acetalizing polyvinyl alcohol with an aldehyde. For example, polyvinyl alcohol can be obtained by saponifying polyvinyl acetate. The degree of saponification of polyvinyl alcohol is generally within the range of 70 to 99.9% by mol.
[0040] The average degree of polymerization of polyvinyl alcohol is preferably greater than or equal to 200, more preferably greater than or equal to 500, even more preferably greater than or equal to 1,500, and even more preferably greater than or equal to 1600, especially preferably greater than or equal to 2600, even more preferably greater than or equal to 2700, preferably less than or equal to 5,000, more preferably less than or equal to equal to 4,000 and even more preferably less than or equal to 3,500. When the average degree of polymerization is greater than or equal to the lower limit above, the penetration resistance of laminated glass is further enhanced. When the average degree of polymerization is less than or equal to the upper limit above, the formation of an interlayer film is facilitated. In particular, when the average degree of polymerization of polyvinyl alcohol is greater than or equal to 1500, it is possible to prevent the appearance of a laminated glass sheet from being deteriorated by poor degassing.
[0041] The average degree of polymerization of polyvinyl alcohol is determined by a method according to JIS K6726 "Test Methods for Polyvinyl Alcohol".
[0042] The number of carbon atoms of the acetal group contained in the polyvinyl acetal resin is not particularly limited. The aldehyde used at the time of production of the polyvinyl acetal resin is not particularly limited. It is preferable that the number of carbon atoms of the acetal group in the polyvinyl acetal resin is within the range of 3 to 5, and it is preferable that the number of carbon atoms of the acetal group is 3 or 4. When the number of atoms carbon of the acetal group in the polyvinyl acetal resin is greater than or equal to 3, the glass transition temperature of the film between layers is sufficiently lowered.
[0043] The aldehyde is not particularly limited. Generally speaking, an aldehyde with 1 to 10 carbon atoms is suitably used as the aforementioned aldehyde. Examples of the aldehyde having 1 to 10 carbon atoms include formaldehyde, acetaldehyde, propionaldehyde, n-butyraldehyde, isobutyraldehyde, n-valeraldehyde, 2-ethylbutyraldehyde, n-hexylaldehyde, n-octylaldehyde, n-nonylaldehyde, n-decylaldehyde, benzaldehyde , and the like. Of these, propionaldehyde, n-butyraldehyde, isobutyraldehyde, n-hexylaldehyde or n-valeraldehyde are preferred, propionaldehyde, n-butyraldehyde or isobutyraldehyde are most preferred, and n-butyraldehyde is most preferred of all. One kind of aldehyde can be used alone, and two or more kinds of aldehyde can be used in combination.
[0044] The hydroxyl group content (the amount of hydroxyl groups) of the polyvinyl acetal resin (1) is preferably greater than or equal to 17 mol%, more preferably greater than or equal to 20% mol , even more preferably greater than or equal to 22% by mol, preferably less than or equal to 30% by mol, more preferably less than 27% by mol and even more preferably less than or equal to 25% by mol. When the hydroxyl group content is greater than or equal to the lower limit above, the interlayer film adhesion strength is further enhanced. In particular, when the hydroxyl group content of the polyvinyl acetal resin (1) is greater than or equal to 20% by mol, the resin is high in reaction efficiency and is excellent in productivity and, furthermore, when less than than 27% by mol, the sound insulating properties of laminated glass are further enhanced. Furthermore, when the hydroxyl group content is less than or equal to the upper limit above, the flexibility of the film between layers is enhanced and manipulation of the film between layers is facilitated.
[0045] The hydroxyl group content of each of the polyvinyl acetal resin (2) and the polyvinyl acetal resin (3) is preferably greater than or equal to 25% by mol, more preferably greater than or equal to 28% by mol, preferably less than or equal to 35% by mol and more preferably less than or equal to 32% by mol. When the hydroxyl group content is greater than or equal to the lower limit above, the interlayer film adhesion strength is further enhanced. Furthermore, when the hydroxyl group content is less than or equal to the upper limit above, the flexibility of the film between layers is enhanced and manipulation of the film between layers is facilitated.
[0046] The hydroxyl group content of the polyvinyl acetal resin is a molar fraction, represented as a percentage, obtained by dividing the amount of ethylene groups to which the hydroxyl group is attached by the total amount of ethylene groups in the main chain. For example, the amount of ethylene groups to which the hydroxyl group is attached can be measured in accordance with JIS K6726 "Test Methods for Polyvinyl Alcohol" to be determined.
[0047] The degree of acetylation (the amount of acetyl groups) of the polyvinyl acetal resin (1) is preferably greater than or equal to 0.01% by mol, more preferably greater than or equal to 0.1 mol%, even more preferably greater than or equal to 7 mol%, more preferably greater than or equal to 9 mol%, preferably less than or equal to 30% mol, more preferably less than or equal to 25% by mol and even more preferably less than or equal to 15% by mol. When the degree of acetylation is greater than or equal to the lower limit above, the compatibility between the polyvinyl acetal resin and a plasticizer is enhanced. When the degree of acetylation is less than or equal to the upper limit above with respect to interlayer film and laminated glass, its moisture resistance is enhanced. In particular, when the degree of acetylation of the polyvinyl acetal resin (1) is greater than or equal to 0.1 mol% and less than or equal to 25% mol, the laminated glass has a more resistance to penetration. great.
[0048] The degree of acetylation of each of the polyvinyl acetal resin (2) and the polyvinyl acetal resin (3) is preferably greater than or equal to 0.01% by mol, more preferably greater than or equal to 0.5% by mol, preferably less than or equal to 10% by mol and even more preferably less than or equal to 2% by mol. When the degree of acetylation is greater than or equal to the lower limit above, the compatibility between the polyvinyl acetal resin and a plasticizer is enhanced. When the degree of acetylation is less than or equal to the upper limit above with respect to interlayer film and laminated glass, its moisture resistance is enhanced.
[0049] The degree of acetylation is a molar fraction, represented as a percentage, obtained by dividing a value obtained by subtracting the amount of ethylene groups to which the acetal group is attached and the amount of ethylene groups to which the hydroxyl group is attached from the total amount of ethylene groups in the main chain by the total amount of ethylene groups in the main chain. For example, the amount of ethylene groups to which the acetal group is attached can be measured according to JIS K6728 "Test Methods for Polyvinyl Butyral".
[0050] The degree of acetalization of the polyvinyl acetal resin (1) (the degree of butyralization in the case of a polyvinyl butyral resin) is preferably greater than or equal to 47 mol%, more preferably greater than or equal to 60% by mol, preferably less than or equal to 80% by mol and more preferably less than or equal to 70% by mol. When the degree of acetalization is greater than or equal to the lower limit above, the compatibility between the polyvinyl acetal resin and a plasticizer is enhanced. When the degree of acetalization is less than or equal to the upper limit above, the reaction time required to produce the polyvinyl acetal resin is shortened.
[0051] The degree of acetalization of each of the polyvinyl acetal resin (2) and the polyvinyl acetal resin (3) (the degree of butyralization in the case of a polyvinyl butyral resin) is preferably greater than or equal to to 55% by mol, more preferably greater than or equal to 67% by mol, preferably less than or equal to 75% by mol and more preferably less than or equal to 71% by mol. When the degree of acetalization is greater than or equal to the lower limit above, the compatibility between the polyvinyl acetal resin and a plasticizer is enhanced. When the degree of acetalization is less than or equal to the upper limit above, the reaction time required to produce the polyvinyl acetal resin is shortened.
[0052] The degree of acetalization is a value that expresses the molar fraction determined by dividing the amount of ethylene groups to which the acetal group is attached by the total amount of ethylene groups in the main chain in terms of percentage. The degree of acetalization can be calculated by a method according to JIS K6728 "Test Methods for Polyvinyl Butyral".
[0053] In this regard, it is preferable that the hydroxyl group content (the amount of hydroxyl groups), the degree of acetalization (the degree of butyralization) and the degree of acetylation are calculated from the results measured by a method accordingly to JIS K6728 "Test Methods for Polyvinyl Butyral". In this context, a method according to ASTM standard D1396-92 and JIS K6728 standard can be used. In the case where the polyvinyl acetal resin is a polyvinyl butyral resin, the hydroxyl group content (the amount of hydroxyl groups), the degree of acetalization (the degree of butyralization) and the degree of acetylation can be calculated from the results measured by a method according to JIS K6728 "Test Methods for Polyvinyl Butyral".
[0054] From the point of view of further improving the penetration resistance of laminated glass, it is preferable that the polyvinyl acetal resin (1) is a polyvinyl acetal resin (A) with a degree of acetylation (A) less than or equal to 8% by mol and a degree of acetalization (a) greater than or equal to 70% by mol or a polyvinyl acetal resin (B) with a degree of acetylation (B) greater than 8% by mol. The polyvinyl acetal resin (1) can be the polyvinyl acetal resin (A) and can be the polyvinyl acetal resin (B).
[0055] The degree of acetylation (a) of the polyvinyl acetal resin (A) is less than or equal to 8% by mol, preferably less than or equal to 7.5% by mol, more preferably less than than or equal to 7 mol%, even more preferably less than or equal to 6.5% by mol, especially preferably less than or equal to 5% by mol, preferably greater than or equal to 0, 1 mol%, more preferably greater than or equal to 0.5% mol, even more preferably greater than or equal to 0.8 mol% and especially preferably greater than or equal to 1% mol. mol. When the degree of acetylation (a) is less than or equal to the upper limit above and greater than or equal to the lower limit above, the transfer of a plasticizing agent can be easily controlled and the sound insulation properties of laminated glass enhanced further.
[0056] The degree of acetalization (a) of the polyvinyl acetal resin (A) is greater than or equal to 70% by mol, preferably greater than or equal to 70.5% by mol, more preferably greater than than or equal to 71% by mol, even more preferably greater than or equal to 71.5% by mol, especially preferably greater than or equal to 72% by mol, preferably less than or equal to 85% by mol, more preferably less than or equal to 83% by mol, even more preferably less than or equal to 81% by mol and especially preferably less than or equal to 79% by mol. When the degree of acetalization (a) is greater than or equal to the lower limit above, the sound insulating properties of laminated glass are further enhanced. When the degree of acetalization (a) is less than or equal to the upper limit above, the reaction time required to produce the polyvinyl acetal resin (A) can be shortened.
[0057] The content ratio (a) of the hydroxyl group of the polyvinyl acetal resin (A) is preferably greater than or equal to 18 mol%, more preferably greater than or equal to 19 mol%, further more preferably greater than or equal to 20% by mol, especially preferably greater than or equal to 21% by mol, preferably less than or equal to 31% by mol, more preferably less than or equal to 30% by mol, even more preferably less than or equal to 29% by mol and especially preferably less than or equal to 28% by mol. When the content ratio (a) of the hydroxyl group is greater than or equal to the lower limit above, the adhesion strength of the first layer is further enhanced. When the content ratio (a) of the hydroxyl group is less than or equal to the upper limit above, the sound insulating properties of laminated glass are further enhanced.
[0058] The degree of acetylation (b) of the polyvinyl acetal resin (B) is greater than 8% by mol, preferably greater than or equal to 9% by mol, more preferably greater than or equal to 9 .5% by mol, even more preferably greater than or equal to 10% by mol, especially preferably greater than or equal to 10.5% by mol, preferably less than or equal to 30% by mol, more preferably less than or equal to 28% by mol, even more preferably less than or equal to 26% by mol and especially preferably less than or equal to 24% by mol. When the degree of acetylation (b) is greater than or equal to the lower limit above, the sound insulation properties of laminated glass are further enhanced. When the degree of acetylation (b) is less than or equal to the upper limit above, the reaction time required to produce the polyvinyl acetal resin (B) can be shortened.
[0059] The degree of acetalization (b) of the polyvinyl acetal resin (B) is preferably greater than or equal to 50% by mol, more preferably greater than or equal to 53% by mol, even more preferably greater than or equal to 55% by mol, especially preferably greater than or equal to 60% by mol, preferably less than or equal to 80% by mol, more preferably less than or equal to 78% by mol mol, even more preferably less than or equal to 76% by mol and especially preferably less than or equal to 74% by mol. When the degree of acetalization (b) is greater than or equal to the lower limit above, the sound insulating properties of laminated glass are further enhanced. When the degree of acetalization (b) is less than or equal to the upper limit above, the reaction time required to produce the polyvinyl acetal resin (B) can be shortened.
[0060] The content ratio (b) of the hydroxyl group of the polyvinyl acetal resin (B) is preferably greater than or equal to 18 mol%, more preferably greater than or equal to 19 mol%, further more preferably greater than or equal to 20% by mol, especially preferably greater than or equal to 21% by mol, preferably less than or equal to 31% by mol, more preferably less than or equal to 30% by mol, even more preferably less than or equal to 29% by mol and especially preferably less than or equal to 28% by mol. When the content ratio (b) of the hydroxyl group is greater than or equal to the lower limit above, the adhesion strength of the first layer is further enhanced. When the content ratio (b) of the hydroxyl group is less than or equal to the upper limit above, the sound insulating properties of laminated glass are further enhanced.
[0061] It is preferable that each of the polyvinyl acetal resin (A) and the polyvinyl acetal resin (B) is a polyvinyl butyral resin. (Plasticizing Agent)
[0062] The first layer contains a plasticizing agent (hereinafter sometimes described as a plasticizing agent (1)). The second layer contains a plasticizing agent (hereinafter sometimes described as a plasticizing agent (2)). It is preferable that the third layer contains a plasticizing agent (hereinafter sometimes described as a plasticizing agent (3)). By using a polyvinyl acetal resin and a plasticizing agent together, the adhesion strength of a layer containing the polyvinyl acetal resin and the plasticizing agent to a laminated glass member or another layer is moderately enhanced. The plasticizing agent is not particularly limited. The plasticizing agent (1), the plasticizing agent (2) and the plasticizing agent (3) can be the same or different from each other. One type of plasticizing agent can be used alone, and two or more types of plasticizer can be used in combination.
[0063] Examples of the plasticizing agent include organic ester plasticizing agents such as a monobasic organic acid ester and a polybasic organic acid ester, organic phosphate plasticizing agents such as an organic phosphate plasticizing agent and an organic phosphite plasticizing agent , and the like. Among these, organic ester plasticizers are preferred. It is preferable that the plasticizing agent is a liquid plasticizing agent.
[0064] Examples of monobasic organic acid ester include a glycol ester obtained by reacting a glycol with a monobasic organic acid, and the like. Examples of glycol include triethylene glycol, tetraethylene glycol, tripropylene glycol, and the like. Examples of monobasic organic acid include butyric acid, isobutyric acid, caproic acid, 2-ethyl butyric acid, heptylic acid, n-octyl acid, 2-ethyl hexanoic acid, n-nonylic acid, decyl acid, and the like.
[0065] Examples of polybasic organic acid ester include an ester compound of a polybasic organic acid and an alcohol having a linear or branched structure of 4 to 8 carbon atoms, and the like. Examples of polybasic organic acid include adipic acid, sebacic acid, azelaic acid, and the like.
Examples of organic ester plasticizing agent include triethylene glycol di-2-ethylpropanoate, triethylene glycol di-2-ethylbutyrate, triethylene glycol di-2-ethylhexanoate, triethylene glycol dicaprylate, di triethylene glycol -n-octanoate, triethylene glycol di-n-heptanoate, tetraethylene glycol di-n-heptanoate, dibutyl sebacate, dioctyl azelate, dibutyl carbitol adipate, di-2-ethylbutyrate of ethylene glycol, 1,3-propylene glycol di-2-ethylbutyrate, 1,4-butylene glycol di-2-ethylbutyrate, diethylene glycol di-2-ethylbutyrate, diethylene di-2-ethylhexanoate glycol, dipropylene glycol di-2-ethylbutyrate, triethylene glycol di-2-ethylpentanoate, tetraethylene glycol di-2-ethylbutyrate, diethylene glycol dicaprylate, dihexyl adipate, dioctyl adipate, adipate of cyclohexyl hexyl, a mixture of heptyl adipate and nonyl adipate, diisononyl adipate, diisodecyl adipate, ad nonyl heptyl ipate, dibutyl sebacate, oil-modified sebacic acid alkyd, a mixture of a phosphoric acid ester and an adipic acid ester, and the like. Organic ester plasticizers other than these may be used. Other adipic acid esters than the adipic acid esters described above can be used.
Examples of organic phosphate plasticizing agent include tributexyethyl phosphate, phenyl isodecyl phosphate, triisopropyl phosphate, and the like.
[0068] It is preferable that the plasticizing agent is a diester plasticizing agent represented by the following (1) below.

[0069] In the formula (1) above, each of R1 and R2 represents an organic group with 2 to 10 carbon atoms, R3 represents an ethylene group, an isopropylene group or an n-propylene group, and p represents a positive integer from 3 to 10. It is preferable that each of R1 and R2 in formula (1) above is an organic group having 5 to 10 carbon atoms, and it is more preferable that each of R1 and R2 is an organic group having 6 to 10 carbon atoms.
It is preferable that the plasticizing agent includes triethylene glycol di-2-ethylhexanoate (3GO), triethylene glycol di-2-ethylbutyrate (3GH) or triethylene glycol di-2-ethylpropanoate, it is more preferable that the plasticizing agent includes triethylene glycol di-2-ethylhexanoate or triethylene glycol di-2-ethylbutyrate, and it is even more preferable for the plasticizing agent to include triethylene glycol di-2-ethylhexanoate.
[0071] The plasticizer content (1) with respect to 100 parts by weight of the polyvinyl acetal resin (1) (hereinafter sometimes described as the content (1)) is preferably greater than or equal to 40 parts by weight, more preferably greater than or equal to 55 parts by weight, preferably less than or equal to 90 parts by weight, and more preferably less than or equal to 85 parts by weight. When the content (1) is greater than or equal to the lower limit above, the flexibility of the film between layers is enhanced and manipulation of the film between layers is facilitated. When the content (1) is less than or equal to the upper limit above, the transparency of the film between layers is further enhanced.
[0072] Each of the plasticizing agent content (2) in relation to 100 parts by weight of the polyvinyl acetal resin (2) (hereinafter, sometimes described as the content (2)) and the plasticizing agent content (3) with respect to 100 parts by weight of the polyvinyl acetal resin (3) (hereinafter, sometimes described as content (3)) is preferably greater than or equal to 30 parts by weight, more preferably greater than or equal to 35 parts by weight, preferably less than or equal to 44 parts by weight and more preferably less than or equal to 42 parts by weight. When each of the content (2) and the content (3) is greater than or equal to the lower limit above, the flexibility of the film between layers is enhanced and manipulation of the film between layers is facilitated. When each of grade (2) and grade (3) is less than or equal to the upper limit above, the penetration resistance of laminated glass is further enhanced.
[0073] From the standpoint of further making an opening more difficult to be generated in an end part of the laminated glass sheet, it is preferable that the content (1) is greater than the content (2) and it is preferable that the content (1) is greater than content (3).
[0074] From the point of view also of highlighting the resistance to penetration of laminated glass, each of the absolute value of the difference between content (1) and content (2) and the absolute value of the difference between content (1) and the content (3) is preferably greater than or equal to 10 parts by weight and more preferably greater than or equal to 20 parts by weight. Each of the absolute value of the difference between grade (1) and grade (2) and the absolute value of the difference between grade (1) and grade (3) is preferably less than or equal to 50 parts in Weight. (Hindered Amine Light Stabilizer)
[0075] The first layer contains a hindered amine light stabilizer. The hindered amine light stabilizer contained in the first layer is a hindered amine light stabilizer which has an alkyl group bonded to the nitrogen atom of a piperidine structure or an alkoxy group bonded to the nitrogen atom of a piperidine structure (henceforth hereafter sometimes described as a hindered amine light stabilizer (X)). Each of the second layer and the third layer may contain a hindered amine light stabilizer, and may not contain a hindered amine light stabilizer. In the case where the second layer and the third layer contain a hindered amine light stabilizer, it is preferable that the hindered amine light stabilizer contained in the second layer and the third layer is a hindered amine light stabilizer (X) which has an alkyl group bonded to the nitrogen atom of a piperidine structure or an alkoxy group bonded to the nitrogen atom of a piperidine structure. One type of hindered amine light stabilizer (X) can be used alone, and two or more types of it can be used in combination.
[0076] It is preferable that the hindered amine light stabilizer (X) is a hindered amine light stabilizer having an alkyl group attached to the nitrogen atom of a piperidine structure, and it is also preferable that the light stabilizer of hindered amine (X) is a hindered amine light stabilizer that has an alkoxy group attached to the nitrogen atom of a piperidine structure.
[0077] Examples of the hindered amine light stabilizer that has an alkyl group attached to the nitrogen atom of a piperidine structure include TINUVIN 765, TINUVIN 622SF, ADK STAB LA-52, and the like.
[0078] Examples of the hindered amine light stabilizer that has an alkoxy group attached to the nitrogen atom of a piperidine structure include TINUVIN XT-850FF, TINUVIN XT-855FF, ADK STAB LA-81, and the like.
[0079] From the viewpoints still of making an opening difficult to be generated in an end part of the laminated glass sheet and also of suppressing an increase in the YI value measured in the end part of the laminated glass sheet, the molecular weight of the hindered amine light stabilizer (X) is preferably less than or equal to 2,000, more preferably less than or equal to 1,000 and most preferably less than or equal to 700.
[0080] At 100% by weight of the first layer, the content of hindered amine light stabilizer (X) is preferably greater than or equal to 0.01% by weight, more preferably greater than or equal to 0 0.05% by weight, preferably less than or equal to 0.5% by weight and more preferably less than or equal to 0.3% by weight. When the content of hindered amine light stabilizer (X) is greater than or equal to the lower limit above and less than or equal to the upper limit above, an opening is more difficult to generate in an end portion of the sheet. laminated glass and an increase in the YI value measured at the edge of the laminated glass sheet can also be suppressed.
[0081] The first layer may contain a hindered amine light stabilizer with the exception of the hindered amine light stabilizer (x). However, it is good to leave the content of a hindered amine light stabilizer with the exception of the hindered amine light stabilizer (X) in the first smaller layer, and it is preferable that the first layer does not contain a hindered amine light stabilizer which not the hindered amine light stabilizer (X). At 100% by weight of the first layer, the content of a hindered amine light stabilizer with the exception of the hindered amine light stabilizer (X) is preferably less than or equal to 0.2% by weight and more preferably less than or equal to 0.1% by weight. (Oxidation inhibitor)
[0082] It is preferable that each of the first layer, the second layer and the third layer contain an oxidation inhibitor. One type of oxidation inhibitor can be used alone, and two or more types of it can be used in combination.
[0083] Examples of the oxidation inhibitor include an oxidation inhibitor that includes a phenol skeleton, an oxidation inhibitor that contains sulfur, an oxidation inhibitor that contains phosphorus, and the like.
[0084] From the standpoint of further suppressing an increase in the YI value measured at the end portion of the laminated glass sheet, it is preferable that the oxidation inhibitor be an oxidation inhibitor that includes a phenol skeleton or an oxidation inhibitor which contains phosphorus, and it is more preferable that the oxidation inhibitor is an oxidation inhibitor which includes a phenol skeleton.
[0085] Examples of oxidation inhibitors that include a phenol skeleton include 2,6-di-t-butyl-p-cresol (BHT), butylated hydroxy anisole (BHA), 1,6-di-t-butyl- 4-ethyl phenol, β-(3,5-di-t-butyl-4-hydroxyphenyl) propionate, 2,2'-methylene bis-(4-methyl-6-butylphenol), 2,2'- methylene bis-(4-ethyl-6-t-butylphenol), 4,4'-butylidene-bis-(3-methyl-6-t-butylphenol), 1,1,3-tris-(2-methyl-hydroxy) -5-t-butylphenyl)butane, tetrakis[methylene-3-(3',5'-butyl-4-hydroxyphenyl)propionate]methane, 1,3,3-tris-(2-methyl-4-hydroxy-5 -t-butylphenol)butane, 1,3,5-trimethyl-2,4,6-tris(3,5-di-t-butyl-4-hydroxybenzyl)benzene, bis(3,3' acid glycol ester -t-butylphenol)butyric acid, bis(3-t-butyl-4-hydroxy-5-methyl benzene propanoic acid)ethylene bis(oxyethylene, and the like.
Examples of phosphorus-containing oxidation inhibitor include tridecyl phosphite, tris(tridecyl) phosphite, triphenyl phosphite, trinonylphenyl phosphite, bis(tridecyl) pentaerythritol diphosphite, bis( decyl)pentaerythritol, tris(2,4-di-t-butylphenyl) phosphite, bis(2,4-di-t-butyl-6-methylphenyl)ethyl ester phosphorous acid, tris(2 phosphite) ,4-di-t-butylphenyl), 2,2'-methylenebis(4,6-di-t-butyl-1-phenyloxy)(2-ethylhexyloxy)phosphorus, and the like.
[0087] From the standpoint of further suppressing an increase in the YI value measured at the end portion of the laminated glass sheet, the molecular weight of the oxidation inhibitor is preferably greater than or equal to 200, more preferably greater than than or equal to 300, even more preferably greater than or equal to 500 and preferably less than or equal to 1,500.
[0088] In 100% by weight of a layer containing the oxidation inhibitor, the content of the oxidation inhibitor is preferably greater than or equal to 0.1% by weight, preferably less than or equal to 2% by weight and more preferably less than or equal to 1.8% by weight. When the oxidation inhibitor content is greater than or equal to the lower limit above and less than or equal to the upper limit above, an opening is even more difficult to generate in an end portion of the laminated glass sheet and an increase in the YI value measured at the end part of the laminated glass sheet can also be suppressed. (Metal/Metal salt)
[0089] It is preferable that the interlayer film includes at least one kind of the first metal atom selected from the group consisting of an alkali metal, zinc and aluminum. The interlayer film does not or does not include an alkaline earth metal. For example, in the case where the first layer is a surface layer, it is preferable that each of the first metal atom and the alkaline earth metal is contained in the first layer. It is preferable that each of the first metal atom and the alkaline earth metal is contained in the second layer. It is preferable that each of the first metal atom and the alkaline earth metal is contained in the third layer. Through the use of the first metal atom and alkaline earth, the control of the adhesion capability between a laminated glass member and the interlayer film or the adhesion capability between the respective layers in the interlayer film is facilitated. Each of the first metal atom and the alkaline earth metal can be in the state of being a metal salt (hereinafter sometimes described as a metal (M) salt) to be mixed.
[0090] It is preferable that the metal salt (M) contains at least one kind of metal selected from the group consisting of Li, Na, K, Rb, Cs, Mg, Ca, Sr and Ba. It is preferable that the interlayer film includes at least one type of metal between K and Mg.
[0091] Furthermore, it is more preferable that the metal salt (M) is an alkali metal salt of an organic acid having 2 to 16 carbon atoms or an alkaline earth salt of an organic acid having 2 to 16 carbon atoms, and it is more preferable that the metal (M) salt is a magnesium carboxylate having 2 to 16 carbon atoms or a potassium carboxylate having 2 to 16 carbon atoms.
[0092] Although magnesium carboxylate having 2 to 16 carbon atoms and potassium carboxylate having 2 to 16 carbon atoms are not particularly limited, examples thereof include magnesium acetate, potassium acetate, propionate magnesium, potassium propionate, magnesium 2-ethylbutanoate, potassium 2-ethylbutanoate, magnesium 2-ethylhexanoate, potassium 2-ethylhexanoate, and the like.
[0093] In the case where the interlayer film includes the first metal atom, each of the content of the first metal atom in the interlayer film, the alkali metal content in the first layer, the content of the first metal atom in the second layer and the content of the second metal atom in the third layer is preferably greater than or equal to 5 ppm, more preferably greater than or equal to 10 ppm, even more preferably greater than or equal to 20 ppm, preferably less than or equal to 300 ppm, more preferably less than or equal to 250 ppm, even more preferably less than or equal to 200 ppm and especially preferably less than or equal to 150 ppm. When the content of the first metal atom is greater than or equal to the lower limit above and less than or equal to the upper limit above, the adhesion capability between a laminated glass member and the film between layers or the adhesion capability between the respective layers in the interlayer film can be somewhat better controlled, and an increase in the YI value measured at the end portion of the laminated glass sheet is also suppressed.
[0094] In the case where the interlayer film includes the alkali metal, each of the alkali metal content in the interlayer film, the alkali metal content in the first layer, the alkali metal content in the second layer and the alkali metal content. alkali metal in the third layer is preferably greater than or equal to 5 ppm, more preferably greater than or equal to 10 ppm, even more preferably greater than or equal to 20 ppm, preferably less than or equal to at 300 ppm, more preferably less than or equal to 250 ppm, even more preferably less than or equal to 200 ppm and especially preferably less than or equal to 150 ppm. When the alkali metal content is greater than or equal to the lower limit above and less than or equal to the upper limit above, the adhesion capacity between a laminated glass member and the film between layers or the adhesion capacity between the respective layers layers in the interlayer film can be somewhat better controlled, and an increase in the YI value measured at the edge of the laminated glass sheet is also suppressed. (Other ingredients)
[0095] Each of the first layer, the second layer and the third layer may contain additives such as an ultraviolet filtering agent, a flame retardant, an antistatic agent, a pigment, a dye, a force-regulating agent of adhesion, a moisture-resistance improving agent, a fluorescent whitening agent, and an infrared radiation absorber, as needed. One type of these additives can be used alone, and two or more types of them can be used in combination.(Other details of interlayer film for laminated glass)
[0096] From the viewpoints of further making an opening difficult to be generated in an end portion of the laminated glass sheet and also of suppressing an increase in the YI value measured at the end portion of the laminated glass sheet, it is preferable that the value of a first layer alkali titer is a positive value.
[0099] From the standpoint of further improving the sound insulation performance of laminated glass, it is preferable that the glass transition temperature of the first layer is lower than or equal to 20°C. The glass transition temperature of the first layer is preferably higher than or equal to -15°C.
[0100] The interlayer film thickness for laminated glass according to the present invention is not particularly limited. From the standpoint of practicality and from the standpoint of sufficiently enhancing the heat protection properties, the film thickness between layers is preferably greater than or equal to 0.1 mm, more preferably greater than or equal to 0.25 mm, preferably less than or equal to 3 mm and more preferably less than or equal to 1.5 mm. When the film thickness between layers is greater than or equal to the lower limit above, the penetration resistance of laminated glass is enhanced. When the film thickness between layers is lower than or equal to the upper limit above, the transparency of the film between layers is further enhanced.
[0101] The film thickness between layers is defined as T. From the standpoints still of making an opening difficult to be generated in an end part of the laminated glass sheet and also of suppressing an increase in the YI value measured in the part edge of the laminated glass sheet, the thickness of the first layer is preferably greater than or equal to 0.0625T, more preferably greater than or equal to 0.1T, preferably less than or equal to 0.375T and more preferably less than or equal to 0.25T.
[0102] From the viewpoints further of making an opening difficult to be generated in an end part of the laminated glass sheet and also of suppressing an increase in the value of YI measured in the end part of the laminated glass sheet, the thickness of each of the second layer and the third layer is preferably greater than or equal to 0.625T, more preferably greater than or equal to 0.75T, preferably less than or equal to 0.9375T and more preferably less than or equal to 0.9T. Furthermore, when the thickness of each of the second layer and the third layer is greater than or equal to the lower limit above and less than or equal to the upper limit above, it is possible to suppress the bleed of the plasticizing agent.
[0103] From the standpoints further of making an opening difficult to be generated in an end part of the laminated glass sheet and also of suppressing an increase in the YI value measured at the part end of the laminated glass sheet, in the case where the interlayer film is provided with the second layer and the third layer, the total thickness of the second layer and the third layer is preferably greater than or equal to 0.625T, more preferably greater than or equal to 0.75T, preferably less than or equal to 0.9375T and more preferably less than or equal to 0.9T. Furthermore, when the total thickness of the second layer and the third layer is greater than or equal to the lower limit above and less than or equal to the upper limit above, it is possible to suppress plasticizing agent bleed.
[0104] Although the method of producing the interlayer film for laminated glass according to the present invention is not particularly limited, examples thereof include a method of separately forming the respective resin compositions used to constitute the respective layers in respective layers, and then, for example, the respective layers obtained are allowed to be arranged on top of each other, a method which allows the respective resin compositions used to constitute the respective layers to be co-extruded using an extruder and which allows the respective layers to be co-extruded. respective layers are arranged on top of each other, and the like. An extrusion molding production method is preferred, because the method is suitable for continuous production.
[0105] Due to the fact that the interlayer film can be excellent in production efficiency, it is preferable that the respective polyvinyl acetal resins contained in the second layer and the third layer are the same as each other, it is more preferable that the respective polyvinyl acetal resins contained in the second layer and the third layer are equal to each other, it is more preferable that the respective polyvinyl acetal resins contained in the second layer and the third layer polyvinyl acetal contained in the second layer and the third layer are the same as each other, and that the respective plasticizers contained therein are the same as each other, and it is also more preferable that the second layer and the third layer are formed from the same. resin composition than the other. (Laminated glass)
[0106] Figure 2 shows an example of laminated glass prepared with an interlayer film for laminated glass according to an embodiment of the present invention schematically represented as a sectional view.
[0107] The laminated glass 11 shown in Figure 2 is provided with a first laminated glass member 21, a second laminated glass member 22 and an interlayer film 1. The interlayer film 1 is arranged between the first laminated glass member 21 and the second laminated glass member 22 to be pressed.
[0108] The first laminated glass member 21 is arranged on a first surface 1a of the interlayer film 1. The second laminated glass member 22 is arranged on a second surface 1b opposite the first surface 1a of the interlayer film 1. The first laminated glass member 21 is arranged on an outer surface 3a of a second layer 3 of the interlayer film 1. The second laminated glass member 22 is arranged on an outer surface 4a of a third layer 4 of the interlayer film 1.
[0109] As described above, laminated glass according to the present invention is provided with a first laminated glass member, a second laminated glass member and an interlayer film arranged between the first laminated glass member and the second member of laminated glass, and the interlayer film is the interlayer film for laminated glass according to the present invention.
[0110] Examples of the laminated glass member include a glass plate, a PET (polyethylene terephthalate) film, and the like. As laminated glass, laminated glass in which an interlayer film is sandwiched between a glass plate and a PET or other film is included, as well as laminated glass in which an interlayer film is sandwiched between two glass plates . Laminated glass is a laminate provided with a glass plate, and it is preferable that at least one glass plate is used. It is preferable that each of the first laminated glass member and the second laminated glass member is a glass plate or a PET (polyethylene terephthalate) film and that the interlayer film includes at least one glass plate as a first member. of laminated glass or second member of laminated glass. It is especially preferable that both the first laminated glass member and the second laminated glass member are sheets of glass.
[0111] Examples of the glass plate include an inorganic glass sheet and an organic glass sheet. Examples of inorganic glass include floating plate glass, heat absorbing plate glass, heat reflecting plate glass, polished plate glass, figured glass, wire plate glass, and the like. . Organic glass is synthetic resin glass substituted for inorganic glass. Examples of organic glass include a polycarbonate plate, a poly(meth)acrylic resin plate, and the like. Examples of the poly(meth)acrylic resin board include a polymethyl(meth)acrylate board, and the like.
[0112] The thickness of the laminated glass member is preferably greater than or equal to 1 mm, preferably less than or equal to 5 mm and more preferably less than or equal to 3 mm. Furthermore, in the case where the laminated glass member is a glass plate, the thickness of the glass plate is preferably greater than or equal to 1 mm, preferably less than or equal to 5 mm and more preferably less than or equal to 3 mm. In the case where the laminated glass member is a PET film, the thickness of the PET film is preferably greater than or equal to 0.03 mm and preferably less than or equal to 0.5 mm.
[0113] The method of producing laminated glass is not particularly limited. For example, an interlayer film is sandwiched between the first laminated glass member and the second laminated glass member, and the air remaining between the first laminated glass member and the interlayer film and between the second laminated glass member and the interlayer film is removed by allowing the limbs to pass through a pinch roller or by placing the limbs in a rubber bag and allowing the contents to be sucked under reduced pressure. Next, the members are preliminarily bonded together at about 70 to 110°C to obtain a laminate. Then, by placing the laminate in an autoclave or by compressing the laminate, the members are pressed together by compression at about 120 to 150°C and under a pressure of 1 to 1.5 MPa. In this way laminated glass can be obtained.
[0114] Interlayer film and laminated glass can be used for automobiles, rail vehicles, airplanes, ships, buildings, and the like. Interlayer film and laminated glass can also be used for applications other than these applications. It is preferable that the interlayer film and laminated glass are an interlayer film and a laminated glass for vehicles or buildings, and it is more preferable that the interlayer film and laminated glass are an interlayer film and laminated vehicle glass. . Interlayer film and laminated glass can be used for a windshield, side window, rear window or roof glass of an automobile, and the like. Interlayer film and laminated glass are suitably used for automobiles. Interlayer film is used to obtain laminated automobile glass.
[0115] Next, the present invention will be described in more detail with reference to examples. The present invention is not limited to these examples only.
[0116] With regard to the polyvinyl butyral (PVB) resin used in the examples and comparative examples below, the degree of butyralization (the degree of acetalization), the degree of acetylation and the hydroxyl group content were measured by a method according to JIS K6728 "Test Methods for Polyvinyl Butyral". In this respect, even in the measurement examples according to ASTM standard D1396-92, numerical values similar to those obtained by a method according to JIS K6728 "Test methods for polyvinyl butyral" were displayed.
[0117] In addition, the following hindered amine light stabilizers (HALSs) were used in the examples and comparative examples. TINUVIN 765 (available from BASF Japan Ltd., type NC (alkyl group), molecular weight 509 ) TINUVIN 622SF (available from BASF Japan Ltd., type NC (alkyl group), with molecular weight of 1,000 or more) ADK STAB LA-81 (available from ADEKA CORPORATION, type NOR (alkoxy group), with molecular weight of 678)TINUVIN XT-855FF (available from BASF Japan Ltd., type N-OR (alkoxy group))TINUVIN 770DF (available from BASF Japan Ltd., type NH (hydrogen atom), with molecular weight of 481) Hostavin N24 (available from Clariant Japan KK, type NH (hydrogen atom), with a molecular weight of 632) Chimassorb 944FDL (available from BASF Japan Ltd., type NH (hydrogen atom), with a molecular weight of 1,000 or more)
[0118] In addition, the following oxidation inhibitors have been used in the examples and comparative examples.BHT (2,6-di-t-butyl-p-cresol, 220 molecular weight) IRGANOX 1010 (available from BASF Japan Ltd., an oxidation inhibitor that includes a phenol skeleton, with a molecular weight of 1,178)IRGANOX 245 (available from BASF Japan Ltd., an oxidation inhibitor that includes a phenol skeleton, with a molecular weight of 587)ADK STAB AO-40 (available from ADEKA CORPORATION, an oxidation inhibitor that includes a phenol skeleton, with a molecular weight of 383) (Example 1) Preparation of Composition X for the formation of the first layer:
[0119] One hundred parts by weight of a polyvinyl acetal resin (a polyvinyl butyral (PVB) resin, with an average degree of polymerization of polyvinyl alcohol (PVA) of 2,300, a hydroxyl group content of 23.2% by mol , a degree of acetylation of 12.5% by mol, a degree of acetalization of 64.3% by mol), 60 parts by weight of triethylene glycol (3GO) di-2-ethylhexanoate, which is a plasticizer, 0 .2 part by weight of TINUVIN 765 (available from BASF Japan Ltd., type N-alkyl group, molecular weight 509) and 0.2 part by weight of BHT (2,6-di-t-butyl- p-cresol, with a molecular weight of 220) were mixed to obtain Composition X for the formation of a first layer. Preparation of Composition Y for the formation of the second and third layers:
[0120] One hundred parts by weight of a polyvinyl acetal resin (a polyvinyl butyral (PVB) resin, with an average degree of polymerization of polyvinyl alcohol (PVA) of 1,700, a hydroxyl group content of 34.5% by mol , a degree of acetylation of 0.8% by mol, a degree of acetalization of 64.8% by mol), 31.5 parts by weight of triethylene glycol di-2-ethylhexanoate (3GO), which is a plasticizing agent , and a compound containing magnesium in an amount in which its content in the interlayer film becomes 60 ppm, were mixed to obtain Composition Y for the formation of a second layer and a third layer. In this regard, a mixture containing magnesium (magnesium acetate : magnesium 2-ethylbutyrate = 50% by weight : 50% by weight) was used. Preparation of the interlayer film:
[0121] By employing Composition X for the formation of a first layer and Composition Y for the formation of a second layer and a third layer to be coextruded using a coextruder, an interlayer film (800 μm thick) which has a layered structure with a stack of a second layer (350 μm thick)/a first layer (100 μm thick)/a third layer (350 μm thick) was prepared.Preparation of laminated glass:
[0122] The interlayer film (multiple layers) obtained was cut to a size of 8 cm in longitudinal length x 8 cm in transverse length. Then, the interlayer film was sandwiched between two sheets of clear glass (8 cm in longitudinal length x 8 cm in transverse length x 2.5 mm in thickness), held in place for 30 minutes at 90°C and compressed under vacuum with a vacuum laminator to obtain a laminate. As far as the laminate is concerned, the portions of the film between projecting layers of the glass sheet were removed in order to obtain a laminated glass sheet. (Examples 2 to 21 and Comparative Examples 1 to 5)
[0123] An interlayer film and a laminated glass sheet were prepared in the same manner as that in Example 1 except that the type of ingredient contained in the first layer, second layer and third layer and the ingredient content were adjusted to those listed in Tables 1 to 3 below.(Assessment)(1) First layer glass transition temperature
[0124] The kneaded products having the respective compositions of the first layer in the examples and comparative examples were prepared. The obtained kneaded product was compression molded with a compression molding machine in order to obtain a resin film A with an average thickness of 0.35 mm. The resin film A obtained was kept for 2 hours under the condition of 25°C and a relative age of 30%. After standing for 2 hours, its viscoelasticity was measured by means of the "ARES-G2" available from TA Instruments Japan Inc. As a template, a parallel plate with a diameter of 8 mm was used. The measurement was performed under the condition that the temperature is decreased from 100°C to -10°C at a temperature decrease rate of 3°C/minute and under the condition of a frequency of 1 Hz and a demand of 1 %. In the measurement results obtained, the peak temperature of the loss tangent was defined as the glass transition temperature Tg (°C).(2) Second layer and third layer glass transition temperature
[0125] The kneaded products having the respective compositions of the second layer and the third layer in the examples and in the comparative examples were prepared. The obtained kneaded product was compression molded with a compression molding machine to obtain a resin film A with an average thickness of 0.35 mm. The resin film A obtained was kept for 2 hours under the condition of 25°C and a relative age of 30%. After standing for 2 hours, its viscoelasticity was measured by means of "ARES-G2" available from TA Instruments Japan Inc. As a template, a parallel plate with a diameter of 8 mm was used. The measurement was performed under the condition that the temperature is decreased from 100°C to -10°C at a temperature decrease rate of 3°C/minute and under the condition of a frequency of 1 Hz and a demand of 1 %. In the measurement results obtained, the peak temperature of the loss tangent was defined as the glass transition temperature Tg (°C).
[0126] In addition, the glass transition temperature Tg was measured by the following method. After the obtained multilayer interlayer film was stored for 1 month under the condition of a temperature of 23°C and a humidity of 30%, the respective layers (the first layer, the second layer and the third layer) were separated from each other to be isolated from each other. Each layer as an object to be measured, which was compression molded with a compression molding machine and had an average thickness of 0.35 mm, was put to rest for 2 hours under the condition of 25°C and a relative humidity. va of 30%, and was measured for viscoelasticity using "ARE-G2" available from TA Instruments Japan Inc. A parallel plate with a diameter of 8 mm was used as a template, and the measurement was performed under the condition in that the temperature is dropped from 100°C to -10°C at a temperature drop rate of 3°C/minute and under the condition of a frequency of 1 Hz and a demand of 1%. In the measurement results obtained, the peak temperature of the loss tangent was defined as the glass transition temperature Tg (°C). In any of the above methods, the same glass transition temperature Tg was obtained.(3) State of the opening generated in the end part of the laminated glass sheet
[0127] A sheet of laminated glass was irradiated with ultraviolet rays (quartz glass mercury lamp (750 W)) for 2000 hours in accordance with JIS R3205 when using an ultraviolet irradiation device ("HLG-2S" " available from Suga Test Instruments Co., Ltd.). After testing, the end portion of the laminated glass sheet was observed to assess the state of an opening generated in the end portion of the laminated glass sheet. The opening status was judged according to the following criteria. Criteria for judging the opening status
[0128] O: In the end part of the laminated glass sheet, there is no opening or the opening is generated only within a distance shorter than or equal to 1 mm from the end part in the orthogonal inward direction beside the end including the end part.
[0129] x: At the end portion of the laminated glass sheet, the opening extends a distance longer than 1 mm from the end portion in the inward-facing direction orthogonal to the side of the end including the end portion. (4) ΔYI value measured at the end part of the laminated glass sheet
[0130] The obtained laminated glass sheet was measured for the YI value (the yellowing index, the yellow index) by a transmission method according to the JIS K7105 standard using a spectrophotometer ("U-4100" available with Hitachi High- Technologies Corporation).
[0131] The end portion of the laminated glass sheet was measured for the initial YI value. Then, the laminated glass sheet was heated for 4 weeks at 100°C. After heating, the end portion of the laminated glass sheet was measured for the YI value after heating. In this regard, the area of the Y-value measurement was defined as an area within a distance of 5 mm from the end portion in the inward-facing direction orthogonal to the side of the end including the end portion. The absolute value of the difference between the initial YI value and the YI value after heating was set to ΔYI to be determined. The value of ΔYI was judged according to the following criteria. Criteria for judging the value of ΔYIO: The value of ΔYI is less than or equal to 20.x: The value of ΔYI is greater than 20.5: ) Properties sound isolation
[0132] The laminated glass was excited by means of a vibration generator for a damping test ("Vibration exciter G21-005D" available from SHINKEN CO., LTD.) to obtain the vibration characteristics, the vibration characteristics were amplified by a mechanical impedance measuring device ("XG-81" available from RION Co., Ltd.), and the vibration spectrum was analyzed by an FFT spectrum analyzer ("FFT analyzer HP3582A" available from Yokogawa Electric Corporation).
[0132] The results are shown in Tables 1 to 3 below. With regard to the evaluation for sound insulating properties, all laminated glass sheets in Examples 1 to 21 are excellent in sound insulating properties.






[0133] In Examples 1 to 21, the glass transition temperature of the second layer and the third layer is higher than or equal to 32°C. As contrasted with Examples 1 to 21, only the type of polyvinyl acetal resin was changed so that the glass transition temperature of the second layer and the third layer became lower than 32°C to obtain the respective films between layers, and the respective interlayer films were used for preparing the laminated glass sheets. As a result, with respect to laminated glass sheets prepared in this way, compared to laminated glass sheets prepared with the interlayer films in Examples 1 to 21, there is a tendency for an opening to be easy to be generated in a part. of the laminated glass sheet, and there is a tendency for the YI value measured at the end portion of the laminated glass sheet to be increased.EXPLANATION OF SYMBOLS6: Film between layers1a: First surface1b: Second surface7: First layer2a: First surface2b : Second surface8: Second layer3a: Outer surface9: Third layer4a: Outer surface11: Laminated glass21: First laminated glass member22: Second laminated glass member

权利要求:
Claims (12)
[0001]
1. Interlayer film for laminated glass, characterized in that it comprises a first layer that contains a polyvinyl acetal resin and a plasticizing agent and a second layer that is arranged on one side of the first surface of the first layer and contains a resin. polyvinyl acetal and a plasticizing agent, wherein the first layer also contains a hindered amine light stabilizer having an alkyl group bonded to the nitrogen atom of a piperidine structure or an alkoxy group bonded to the nitrogen atom of a piperidine structure , and the second layer has a glass transition temperature higher than or equal to 32°C.
[0002]
2. Interlayer film for laminated glass according to claim 1, characterized in that at least one first metal atom selected from the group consisting of an alkaline earth metal, zinc and aluminum is included in the interlayer film, a alkali metal is not included or is included in the interlayer film, and the content of the first metal atom in the interlayer film is less than or equal to 150 ppm.
[0003]
3. Interlayer film for laminated glass according to claim 1 or 2, characterized in that the content of plasticizer contained in the first layer in relation to 100 parts by weight of the polyvinyl acetal resin contained in the first layer is greater than that the content of plasticizer contained in the second layer is relative to 100 parts by weight of the polyvinyl acetal resin contained in the second layer.
[0004]
4. Interlayer film for laminated glass according to any one of claims 1 to 3, characterized in that the polyvinyl acetal resin contained in the first layer is obtained by acetalizing a polyvinyl alcohol with a higher average degree of polymerization than that or equal to 1,500.
[0005]
5. Interlayer film for laminated glass according to any one of claims 1 to 4, characterized in that the degree of acetylation of the polyvinyl acetal resin contained in the first layer is greater than or equal to 0.1% in mol and less than or equal to 25% by mol, and the hydroxyl group content of the polyvinyl acetal resin contained in the first layer is greater than or equal to 20% by mol and less than 30% by mol.
[0006]
6. Interlayer film for laminated glass according to any one of claims 1 to 5, characterized in that the glass transition temperature of the first layer is less than or equal to 20°C.
[0007]
7. Interlayer film for laminated glass according to any one of claims 1 to 6, characterized in that the first layer contains an oxidation inhibitor that has a molecular weight of greater than or equal to 250 and includes a skeleton of phenol.
[0008]
8. Interlayer film for laminated glass according to any one of claims 1 to 7, characterized in that the molecular weight of the hindered amine light stabilizer is less than or equal to 1,000.
[0009]
9. Interlayer film for laminated glass according to any one of claims 1 to 8, characterized in that it also comprises a third layer which is arranged on a second surface side opposite the first surface of the first layer and which contains a resin of polyvinyl acetal and a plasticizing agent.
[0010]
10. Interlayer film for laminated glass according to claim 9, characterized in that the glass transition temperature of the third layer is greater than or equal to 32°C.
[0011]
11. Interlayer film for laminated glass according to any one of claims 1 to 10, characterized in that it is used to obtain laminated glass for an automobile.
[0012]
12. Laminated glass, characterized in that it comprises a first laminated glass member, a second laminated glass member and an interlayer film for laminated glass as defined in any one of claims 1 to 11, wherein the interlayer film for laminated glass laminated glass is arranged between the first laminated glass member and the second laminated glass member.

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同族专利:

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公开号 | 公开日

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CN105939980A|2016-09-14|

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JPWO2015147302A1|2017-04-13|

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EP3124451A1|2017-02-01|

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JP2016179939A|2016-10-13|

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CN105939979A|2016-09-14|

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JP5946964B2|2016-07-06|

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JP2016047796A|2016-04-07|

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EP3124451B1|2018-08-01|

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EP3124452A1|2017-02-01|

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MX2016012444A|2017-01-06|

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KR20160140581A|2016-12-07|

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WO2015147303A1|2015-10-01|

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RU2681971C2|2019-03-14|

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CN105939980B|2019-03-22|

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JPWO2015147303A1|2017-04-13|

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ZA201606489B|2018-12-19|

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KR20160138378A|2016-12-05|

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RU2016142224A|2018-04-28|

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US20170072665A1|2017-03-16|

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JP5838011B1|2015-12-24|

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RU2016142224A3|2018-07-27|

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BR112016021517A2|2017-08-15|

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EP3124452B1|2018-07-25|

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EP3124451A4|2017-07-05|

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WO2015147302A1|2015-10-01|

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KR102360715B1|2022-02-10|

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US20170217132A1|2017-08-03|

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RU2687704C2|2019-05-15|

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RU2016142220A3|2018-11-07|

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CN105939979B|2019-06-28|

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MX2016012549A|2017-01-09|

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EP3124452A4|2017-06-28|

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RU2016142220A|2018-04-28|

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法律状态:
2020-01-14| B06U| Preliminary requirement: requests with searches performed by other patent offices: procedure suspended [chapter 6.21 patent gazette]|

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2021-06-01| B09A| Decision: intention to grant [chapter 9.1 patent gazette]|

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2021-07-20| B350| Update of information on the portal [chapter 15.35 patent gazette]|

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2021-08-03| B350| Update of information on the portal [chapter 15.35 patent gazette]|

优先权:

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申请号 | 申请日 | 专利标题

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JP2014-069975|2014-03-28|

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JP2014069975|2014-03-28|

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JP2014069976|2014-03-28|

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JP2014-069976|2014-03-28|

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PCT/JP2015/059781|WO2015147302A1|2014-03-28|2015-03-27|Intermediate film for laminated glass, and laminated glass|

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