JP6985259B2 - Molded body and laminated glass - Google Patents

Description

The present invention relates to a molded product that can be suitably used for an interlayer film for laminated glass and the like. The present invention also relates to a laminated glass using the above-mentioned molded product.

The polyvinyl acetal resin is used for various purposes such as an interlayer film for laminated glass in laminated glass, a wash primer for metal treatment, various paints, an adhesive, a resin processing agent, and a ceramic binder. In recent years, the use of polyvinyl acetal resin has expanded to electronic materials and the like.

Even if the laminated glass is damaged by an external impact, the amount of scattered glass fragments is small and the laminated glass is excellent in safety. Therefore, the laminated glass is widely used in automobiles, railroad vehicles, aircraft, ships, buildings and the like. The laminated glass is manufactured by sandwiching an interlayer film for laminated glass between two glass plates.

As an example of the composition used for the interlayer film for laminated glass and the like, Patent Document 1 below discloses a polyvinyl acetal-based resin composition containing a polyvinyl acetal resin and a resin having a crosslinked structure. The composition has a structure in which a resin having a crosslinked structure is dispersed as a dispersed phase in the polyvinyl acetal resin as a continuous phase. When the dynamic viscoelastic spectrum is measured at a frequency of 10 Hz, the composition has a maximum value of the loss tangent derived from the polyvinyl acetal resin at 40 ° C. or higher, and the loss derived from the resin having a crosslinked structure. It has a maximum value of tangent at 10 ° C or lower. The resin having a crosslinked structure is a (meth) acrylic resin having a crosslinked structure.

Patent Document 2 below discloses an interlayer film which is a polymer layer having a glass transition temperature of 33 ° C. or higher. Patent Document 2 describes that the polymer layer is arranged between glass plates having a thickness of 4.0 mm or less.

WO2014 / 050746A1 US2013 / 0236711A1

Patent Document 1 describes that excellent mechanical strength is exhibited in a wide temperature range from low temperature to high temperature. As the mechanical strength, tensile elongation and breaking strength at −20 ° C., 0 ° C., 20 ° C., 40 ° C., and 80 ° C. are measured. In this mechanical strength test, a tensile test is performed at a relatively low speed of 100 mm / min.

For example, laminated glass used in automobiles is subjected to deformation stress at a considerably high speed when an external impact is applied. In addition, laminated glass may be exposed to a low temperature environment. The present inventors have focused on the problem of further improving the fracture strength of a molded body such as an interlayer film against a high-speed deformation stress at a low temperature.

An object of the present invention is to provide a molded product capable of increasing the breaking elongation at low temperature and high speed and increasing the breaking strength at low temperature and high speed. It is also an object of the present invention to provide a laminated glass using the above-mentioned molded body.

According to a broad aspect of the present invention, it contains a polyvinyl acetal resin and a polymer of a polymerizable component containing a (meth) acrylate compound having two or more (meth) acryloyl groups, with respect to 100 parts by weight of the polyvinyl acetal resin. Therefore, a molded product having a polymer content of 85 parts by weight or more and 180 parts by weight or less and having a phase-separated structure is provided.

In a specific aspect of the molded product according to the present invention, a (meth) acrylate compound having two or more (meth) acryloyl groups and a (meth) acryloyl group in 100% by weight of the polymerizable component constituting the polymer are used. The total amount of the polymer compound having a (meth) acryloyl group other than the two or more (meth) acrylate compounds is 50% by weight or more, and the polymer is an acrylic polymer.

In certain aspects of the molded product according to the present invention, the molded product does not contain a plasticizer or contains 10 parts by weight or less of the plasticizer with respect to 100 parts by weight of the polyvinyl acetal resin and the polymer in total. Including in.

In certain aspects of the molded body according to the present invention, the molded body does not contain a plasticizer, or the plasticizer is 5 parts by weight or less based on 100 parts by weight of the polyvinyl acetal resin and the polymer in total. Including in.

In certain aspects of the molded body according to the present invention, the molded body comprises a plasticizer.

In a specific aspect of the molded product according to the present invention, the gel fraction determined by the following formula (X) is 0% by weight or more and 50% by weight or less.

Gel fraction (% by weight) = W2 / W1 × 100 ・ ・ ・ Equation (X)
W1: Weight of the molded product before immersing the molded product in tetrahydrofuran at 23 ° C. W2: Weight of the molded product after immersing the molded product in tetrahydrofuran at 23 ° C. and then taking it out and drying it.

In a specific aspect of the molded product according to the present invention, the polyvinyl acetal resin and the polymer are crosslinked.

In certain aspects of the molded body according to the present invention, the molded body is an interlayer film for laminated glass.

In certain aspects of the molded body according to the present invention, the thickness is 3 mm or less.

In a specific aspect of the molded body according to the present invention, the molded body uses a first glass plate having a thickness of 1.6 mm or less between the first glass plate and the second glass plate. It is placed and used to obtain laminated glass.

In certain aspects of the molded body according to the present invention, the molded body is placed between the first glass plate and the second glass plate and used to obtain a laminated glass, said first glass. The total of the thickness of the plate and the thickness of the second glass plate is 3.5 mm or less.

According to a broad aspect of the present invention, the first laminated glass member, the second laminated glass member, the above-mentioned molded body, and the first laminated glass member and the second laminated glass member are provided. Laminated glass is provided in which the molded body is arranged.

In a specific aspect of the laminated glass according to the present invention, the first laminated glass member is a first glass plate, and the thickness of the first glass plate is 1.6 mm or less.

In a specific aspect of the laminated glass according to the present invention, the first laminated glass member is a first glass plate, the second laminated glass member is a second glass plate, and the first glass. The total of the thickness of the plate and the thickness of the second glass plate is 3.5 mm or less.

The molded product according to the present invention contains a polyvinyl acetal resin and a polymer of a polymerizable component containing a (meth) acrylate compound having two or more (meth) acryloyl groups. In the molded product according to the present invention, the content of the polymer is 85 parts by weight or more and 180 parts by weight or less with respect to 100 parts by weight of the polyvinyl acetal resin. The molded product according to the present invention has a phase-separated structure. Since the molded body according to the present invention has the above-mentioned configuration, it is possible to increase the breaking elongation of the molded body according to the present invention at low temperature and high speed, and to increase the breaking strength at low temperature and high speed. can.

FIG. 1 is a cross-sectional view schematically showing an interlayer film for laminated glass as a molded body according to the first embodiment of the present invention. FIG. 2 is a cross-sectional view schematically showing an interlayer film for laminated glass as a molded body according to a second embodiment of the present invention. FIG. 3 is a cross-sectional view schematically showing an example of a laminated glass using the interlayer film for laminated glass shown in FIG. FIG. 4 is a cross-sectional view schematically showing an example of a laminated glass using the laminated glass interlayer film shown in FIG. 2.

Hereinafter, the present invention will be described in detail.

(Molded body)
The molded product according to the present invention is a polymer of a polymerizable component containing a polyvinyl acetal resin and a (meth) acrylate compound having two or more (meth) acryloyl groups (hereinafter, may be referred to as polymer X). including. The (meth) acrylate compound having two or more (meth) acryloyl groups is a polymerizable compound. The (meth) acrylate compound having two or more (meth) acryloyl groups is used as a part or all of the polymerizable component constituting the polymer X. In the molded product according to the present invention, the polymer X is used as a second resin other than the polyvinyl acetal resin. In the molded product according to the present invention, the content of the polymer X is 85 parts by weight or more and 180 parts by weight or less with respect to 100 parts by weight of the polyvinyl acetal resin.

The molded product according to the present invention has a phase-separated structure.

Since the molded body according to the present invention has the above-mentioned configuration, it is possible to increase the breaking elongation of the molded body according to the present invention at low temperature and high speed, and to increase the breaking strength at low temperature and high speed. can. For example, the breaking elongation and breaking strength of the molded product according to the present invention at −20 ° C. can be increased. In addition, the breaking elongation and breaking strength of the molded product according to the present invention at a high speed of 500 mm / min can be increased.

Further, when a molded body is used as an interlayer film for laminated glass, the molded body is often arranged between a first glass plate and a second glass plate in order to obtain a laminated glass. Even if the thickness of the first glass plate is thin, the use of the molded body according to the present invention provides high low-temperature and high-speed breaking elongation of the molded body and high low-temperature and high-speed breaking strength of the molded body. It is possible to effectively suppress the breakage of the glass and the scattering of the glass plate. Further, even if the thickness of both the first glass plate and the second glass plate is thin, the use of the molded body according to the present invention can sufficiently suppress the breakage of the laminated glass and the scattering of the glass plate. If both the first glass plate and the second glass plate are thick, breakage of the laminated glass and scattering of the glass plate can be further suppressed.

From the viewpoint of increasing the breaking elongation and breaking strength at low temperature and high speed, the content of the polymer X is 85 parts by weight or more and 180 parts by weight or less with respect to 100 parts by weight of the polyvinyl acetal resin. From the viewpoint of further enhancing the breaking elongation and breaking strength at low temperature and high speed, the content of the polymer X is preferably 90 parts by weight or more, preferably 130 parts by weight with respect to 100 parts by weight of the polyvinyl acetal resin. It is less than a part.

The molded product has a phase-separated structure from the viewpoint of increasing the elongation and breaking strength at low temperature and high speed. From the viewpoint of further increasing the breaking elongation and breaking strength at low temperature and high speed, it is preferable that the polymer X is an island portion (domain) in the phase separation structure. It is considered that one of the factors for achieving the above effect in the present invention is that the energy distribution proceeds smoothly due to the phase separation structure.

It is preferable that the polyvinyl acetal resin surrounds the domain, and it is preferable that the polyvinyl acetal resin is a matrix. The phase-separated structure is preferably a co-continuous structure or a sea-island structure. The phase-separated structure may be a co-continuous structure or a sea-island structure. It is preferable that the polyvinyl acetal resin and the polymer X are contained in different phases. It is preferable that the polyvinyl acetal resin and the polymer X form a phase-separated structure. In the case of a sea-island structure, the polyvinyl acetal resin may be a sea portion and the polymer X may be an island portion, and the polymer X may be a sea portion and the polyvinyl acetal resin may be an island portion. good. In the phase-separated structure, the polyvinyl acetal resin may be continuous (may have a continuous structure), and the polymer X may be continuous (may have a continuous structure). ), The polyvinyl acetal resin and the polymer X may form a co-continuous structure. In the phase-separated structure, the polyvinyl acetal resin may be present in a mesh pattern, or the polymer X may be present in a network pattern. Since the effect of the present invention is excellent, it is preferable that the polyvinyl acetal resin and the polymer X have a sea-island structure or a co-continuous structure. That is, in the phase-separated structure, it is preferable that the polyvinyl acetal resin and the polymer X form a sea-island structure or a co-continuous structure.

In the phase separation structure, the average diameter of the islands is preferably 10 nm or more, more preferably 15 nm or more, still more preferably 20 nm or more, particularly preferably 30 nm or more, preferably 13 μm or less, more preferably 10 μm or less, still more preferable. Is 2 μm or less, particularly preferably 1 μm or less. The diameter of each island indicates the maximum diameter, and the average diameter of the islands is obtained by averaging the diameters (maximum diameters) of a plurality of islands.

From the viewpoint of further increasing the breaking elongation and breaking strength at low temperature and high speed, the gel fraction determined by the following formula (X) in the above-mentioned molded body is preferably 0% by weight or more, preferably 50% by weight or less. More preferably, it is 30% by weight or less.

Gel fraction (% by weight) = W2 / W1 × 100 ・ ・ ・ Equation (X)
W1: Weight of the molded product before immersing the molded product in tetrahydrofuran at 23 ° C. W2: Weight of the molded product after immersing the molded product in tetrahydrofuran at 23 ° C. and then taking it out and drying it.

The molded product according to the present invention is suitably used as an interlayer film for laminated glass (hereinafter, may be referred to as an interlayer film). The interlayer film has a one-layer structure or two or more layers. The interlayer film may have a structure of one layer or may have a structure of two or more layers. The interlayer film may have a structure of two layers or may have a structure of three or more layers. The interlayer film comprises a first layer. The interlayer film may be a single-layer interlayer film including only the first layer, or may be a multi-layer intermediate film including the first layer and another layer.

The interlayer film may have a structure of two or more layers, and may include a second layer in addition to the first layer. It is preferable that the interlayer film further includes a second layer. When the interlayer film includes the second layer, the second layer is arranged on the first surface side of the first layer.

The interlayer film may have a structure of three or more layers, and may include a third layer in addition to the first layer and the second layer. It is preferable that the interlayer film further includes a third layer. When the interlayer film includes the second layer and the third layer, the third layer is arranged on the second surface side opposite to the first surface of the first layer. Ru.

The surface of the second layer opposite to the first layer side is preferably a surface on which a laminated glass member or a glass plate is laminated. The thickness of the glass plate laminated on the second layer is preferably 1.6 mm or less, more preferably 1.3 mm or less. The second surface opposite to the first surface of the first layer (the surface on the second layer side) may be a surface on which a laminated glass member or a glass plate is laminated. The thickness of the glass plate laminated on the first layer is preferably 1.6 mm or less, more preferably 1.3 mm or less. The surface of the third layer opposite to the first layer side is preferably a surface on which a laminated glass member or a glass plate is laminated. The thickness of the glass plate laminated on the third layer is preferably 1.6 mm or less, more preferably 1.3 mm or less.

The interlayer film is arranged between the first glass plate and the second glass plate, and is suitably used for obtaining laminated glass. Since the flexural rigidity, breaking elongation and breaking strength can be sufficiently increased due to the interlayer film, the total of the thickness of the first glass plate and the thickness of the second glass plate is preferably 3. It is 5 mm or less, more preferably 3 mm or less. The interlayer film is arranged between the first glass plate and the second glass plate, and is suitably used for obtaining laminated glass. Since the bending rigidity, breaking elongation and breaking strength can be sufficiently increased due to the interlayer film, the interlayer film is a first glass having a thickness of 1.6 mm or less (preferably 1.3 mm or less). Using a plate, it is disposed between the first glass plate and the second glass plate, and is suitably used for obtaining laminated glass. The interlayer film comprises a first glass plate having a thickness of 1.6 mm or less (preferably 1.3 mm or less) and a second glass plate having a thickness of 1.6 mm or less (preferably 1.3 mm or less). It is more preferably used to obtain laminated glass by being arranged between the first glass plate and the second glass plate. Also in this case, the bending rigidity, the breaking elongation and the breaking strength can be sufficiently increased due to the interlayer film.

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

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

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

It should be noted that other layers may be arranged between the second layer 2 and the first layer 1 and between the first layer 1 and the third layer 3, respectively. It is preferable that the second layer 2 and the first layer 1 and the first layer 1 and the third layer 3 are directly laminated, respectively. Examples of the other layer include a layer containing polyethylene terephthalate and the like.

FIG. 2 is a cross-sectional view schematically showing an interlayer film for laminated glass as a molded body according to a second embodiment of the present invention.

The interlayer film 11A shown in FIG. 2 is a single-layer interlayer film having a one-layer structure. The interlayer film 11A is the first layer. The interlayer film 11A is used to obtain a laminated glass. The interlayer film 11A is an interlayer film for laminated glass.

Hereinafter, the details of the first layer, the second layer, and the third layer constituting the molded product, and each of the first layer, the second layer, and the third layer. The details of the ingredients will be described.

(resin)
The molded product contains a polyvinyl acetal resin and a polymer X as a polymerizable component containing a (meth) acrylate compound having two or more (meth) acryloyl groups. It is preferable that the first layer, the second layer and the third layer each contain a polyvinyl acetal resin. It is preferable that the first layer, the second layer and the third layer each contain the polymer X. As the polyvinyl acetal resin, only one kind may be used, or two or more kinds may be used in combination. As the polymer X, only one kind may be used, or two or more kinds may be used in combination.

From the viewpoint of effectively enhancing the affinity between the resin component and the plasticizer and effectively enhancing the penetration resistance, the polyvinyl acetal resin is a polyvinyl acetatetal resin, a polyvinyl butyral resin, a polyvinylbenzyl acetal resin or a polyvinylcumin acetal. It is preferably a resin. From the viewpoint of further increasing the bending rigidity at 40 ° C., the polyvinyl acetal resin is preferably a polyvinyl acetal resin. As used herein, the polyvinyl acetal resin includes acetalized resins, benzyl acetalized resins and cumin acetalized resins.

From the viewpoint of further enhancing the breaking elongation and breaking strength at low temperature and high speed, the molded product may be a polyolefin resin, an acrylic polymer, a urethane polymer, a silicone polymer, rubber, or vinyl acetate as the polymer X. It preferably contains a coalescence, more preferably an acrylic polymer. The acrylic polymer is a polymer obtained by using 50% by weight or more of a polymerizable compound having a (meth) acryloyl group as a polymerizable component.

A (meth) acrylate compound having two or more (meth) acryloyl groups and a (meth) acrylate compound having two or more (meth) acryloyl groups in 100% by weight of the polymerizable component constituting the polymer X (meth). Meta) The total amount with the polymerizable compound having an acryloyl group is defined as the total amount A. From the viewpoint of further increasing the breaking elongation and breaking strength at low temperature and high speed, the total amount A is preferably 50% by weight or more, more preferably 60% by weight or more, still more preferably 70% by weight or more, and particularly preferably 70% by weight or more. 80% by weight or more, most preferably 90% by weight or more. When the total amount A is 50% by weight or more, the obtained polymer X is an acrylic polymer.

Examples of the (meth) acrylate compound having two or more (meth) acryloyl groups include diethylene glycol di (meth) acrylate, dipropylene glycol di (meth) acrylate, triethylene glycol di (meth) acrylate, and tripropylene glycol di (meth). ) Acrylate, Tetraethylene glycol di (meth) acrylate, Tetrapropylene glycol di (meth) acrylate, Polyethylene glycol di (meth) acrylate, Polypropylene glycol di (meth) acrylate, 3-Methyl-1,5-pentanediol di (meth) ) Acrylate, 1,6-hexanediol di (meth) acrylate, 2-butyl-2-ethyl-1,3-propanediol di (meth) acrylate, 1,9-nonanediol di (meth) acrylate, dimethylol-tri Bifunctional (meth) acrylate compounds such as cyclodecandi (meth) acrylate, neopentyl glycol di (meth) acrylate hydroxypivalate, tritetramethylene glycol di (meth) acrylate, and ethoxylated bisphenol A di (meth) acrylate; Pentaerythritol tri (meth) acrylate, trimethylolpropantri (meth) acrylate, trimethylol ethanetri (meth) acrylate di (meth) acrylate, dipentaerythritol tri (meth) acrylate, ε-caprolactone-modified tris- (2- (2- ( Trifunctional (meth) acrylate compounds such as meta) acryloxyethyl) isocyanurate, tris phosphate [2-((meth) acryloyloxy) ethyl]; pentaerythritol tetra (meth) acrylate, dipentaerythritol tetra (meth). Examples thereof include tetrafunctional or higher functional (meth) acrylate compounds such as acrylate, ethoxylated pentaerythritol tetra (meth) acrylate, dipentaerythritol penta (meth) acrylate, and dipentaerythritol hexa (meth) acrylate.

The (meth) acrylate compound having two or more (meth) acryloyl groups may be an epoxy (meth) acrylate compound and a urethane (meth) acrylate compound.

The polymer X is preferably a polymer of a polymerizable component containing a (meth) acrylic acid ester. The polymer X is preferably a poly (meth) acrylic acid ester.

The poly (meth) acrylic acid ester is not particularly limited. Examples of the poly (meth) acrylic acid ester include methyl poly (meth) acrylate, ethyl poly (meth) acrylate, n-propyl poly (meth) acrylate, i-propyl poly (meth) acrylate, and poly. N-butyl (meth) acrylate, i-butyl poly (meth) acrylate, t-butyl poly (meth) acrylate, 2-ethylhexyl poly (meth) acrylate, 2-hydroxyethyl poly (meth) acrylate, 2-Hydroxypropyl poly (meth) acrylate, 4-hydroxybutyl poly (meth) acrylate, glycidyl poly (meth) acrylate, octyl poly (meth) acrylate, propyl poly (meth) acrylate, poly (meth) 2-ethyloctyl acrylate, nonyl poly (meth) acrylate, isononyl poly (meth) acrylate, decyl poly (meth) acrylate, isodecyl poly (meth) acrylate, lauryl poly (meth) acrylate, poly (meth) ) Isotetradecyl acrylate, cyclohexyl poly (meth) acrylate, isobornyl poly (meth) acrylate, benzyl poly (meth) acrylate and the like. The (meth) acrylic acid having a polar group and the (meth) acrylic acid ester include (meth) acrylic acid, 2-hydroxyethyl (meth) acrylic acid, 4-hydroxybutyl (meth) acrylic acid, and the like. Examples thereof include (meth) glycidyl acrylate. Polyacrylic acid ester is preferable because the temperature showing the maximum value of tan δ can be easily controlled within an appropriate range in the dynamic viscoelastic spectrum, and ethyl polyacrylate, n-butyl polyacrylate, and polyacrylic acid are preferable. 2-Ethylhexyl acid or octyl polyacrylate are more preferred. By using these preferable poly (meth) acrylic acid esters, the balance between the productivity of the molded product and the characteristics of the molded product is further improved. Only one kind of the poly (meth) acrylic acid ester may be used, or two or more kinds thereof may be used in combination.

It is preferable that the polyvinyl acetal resin and the polymer X are crosslinked. The molded product may contain the polyvinyl acetal resin and the polymer X as a crosslinked product in which the polyvinyl acetal resin and the polymer X are crosslinked. The thermoplastic resin may have a crosslinked structure. With the crosslinked structure, the shear storage elastic modulus can be controlled, and a molded product having both excellent flexibility and high strength can be produced.

Examples of the method for cross-linking the resin include the following methods. A method in which functional groups that react with each other are introduced into the polymer structure of a resin to form crosslinks. A method of cross-linking using a cross-linking agent having two or more functional groups that react with the functional groups present in the polymer structure of the resin. A method of cross-linking a polymer using a radical generator having a hydrogen abstraction ability such as a peroxide. A method of cross-linking by electron beam irradiation. Since it is easy to control the shear storage elastic modulus and the productivity of the molded body is increased, a method of introducing functional groups that react with each other into the polymer structure of the resin to form a crosslink is preferable.

When the molded product contains a crosslinked product of the polyvinyl acetal resin and the polymer X, a polymerizable component containing a (meth) acrylate compound having two or more (meth) acryloyl groups in the presence of the polyvinyl acetal resin. It is preferable that the step of forming the polymer X by polymerizing and obtaining a molded product is performed. By this step, a structure in which the polyvinyl acetal resin and the polymer X are crosslinked is formed.

The first layer (including a single-layer molded product) preferably contains a thermoplastic resin (hereinafter, may be referred to as a thermoplastic resin (1)). The first layer preferably contains a polyvinyl acetal resin (hereinafter, may be referred to as a polyvinyl acetal resin (1)) as the thermoplastic resin (1). In the case of the single-layer molded body having only the first layer, the molded body contains the polyvinyl acetal resin (1). The second layer preferably contains a thermoplastic resin (hereinafter, may be referred to as a thermoplastic resin (2)). The second layer preferably contains a polyvinyl acetal resin (hereinafter, may be referred to as a polyvinyl acetal resin (2)) as the thermoplastic resin (2). The third layer preferably contains a thermoplastic resin (hereinafter, may be referred to as a thermoplastic resin (3)). The third layer preferably contains a polyvinyl acetal resin (hereinafter, may be referred to as a polyvinyl acetal resin (3)) as the thermoplastic resin (3). The polyvinyl acetal resin (1), the polyvinyl acetal resin (2), and the polyvinyl acetal resin (3) 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) because the sound insulation property is further improved. The thermoplastic resin (1), the thermoplastic resin (2), and the thermoplastic resin (3) may be the same or different. The polyvinyl acetal resin (1), the polyvinyl acetal resin (2), and the polyvinyl acetal resin (3) may be used alone or in combination of two or more. Only one kind of the thermoplastic resin (1), the thermoplastic resin (2), and the thermoplastic resin (3) may be used, or two or more kinds thereof may be used in combination.

Examples of the thermoplastic resin include polyvinyl acetal resin, polyacrylic resin, ethylene-vinyl acetate copolymer resin, ethylene-acrylic acid copolymer resin, polyurethane resin, polyvinyl alcohol resin and the like. Thermoplastic resins other than these may be used.

The polyvinyl acetal resin is preferably an acetal product of polyvinyl alcohol. The polyvinyl alcohol can be obtained, for example, by saponifying polyvinyl acetate. The saponification degree of the polyvinyl alcohol is generally 70 to 99.9 mol%.

The average degree of polymerization of the polyvinyl alcohol (PVA) is preferably 200 or more, more preferably 500 or more, still more preferably 1500 or more, still more preferably 1600 or more, particularly preferably 2600 or more, most preferably 2700 or more, preferably 2700 or more. It is 5000 or less, more preferably 4000 or less, still more preferably 3500 or less. When the average degree of polymerization is at least the above lower limit, the penetration resistance and bending rigidity of the laminated glass are further increased. When the average degree of polymerization is not more than the above upper limit, molding of the molded product becomes easy.

The average degree of polymerization of polyvinyl alcohol is determined by a method based on JIS K6726 "polyvinyl alcohol test method".

The acetal group in the polyvinyl acetal resin preferably has 2 to 10 carbon atoms, more preferably 2 to 5, and even more preferably 2, 3 or 4. Further, it is preferable that the acetal group in the polyvinyl acetal resin has 2 or 4 carbon atoms, and in this case, the production of the polyvinyl acetal resin is efficient.

As the aldehyde, generally, an aldehyde having 1 to 10 carbon atoms is preferably used. Examples of the aldehyde having 1 to 10 carbon atoms include formaldehyde, acetaldehyde, propionaldehyde, n-butylaldehyde, isobutylaldehyde, n-barrel aldehyde, 2-ethylbutylaldehyde, n-hexylaldehyde, and n-octylaldehyde. Examples thereof include n-nonylaldehyde, n-decylaldehyde, cuminaldehyde, and benzaldehyde. Acetaldehyde, propionaldehyde, n-butyraldehyde, isobutyraldehyde, n-hexyl aldehyde or n-barrel aldehyde are preferred. Acetaldehyde, propionaldehyde, n-butyraldehyde, isobutylaldehyde or n-barrelaldehyde are more preferred, and acetaldehyde, n-butyraldehyde or n-barrelaldehyde are even more preferred. Only one kind of the above aldehyde may be used, or two or more kinds may be used in combination.

When the polyvinyl acetal resin (1) is used as a part of a single-layer molded body, the hydroxyl group content (hydroxyl group amount) of the polyvinyl acetal resin (1) is preferably in the following range. The hydroxyl group content (hydroxyl group amount) of the polyvinyl acetal resin (1) is preferably 25 mol% or more, more preferably 28 mol% or more, more preferably 30 mol% or more, still more preferably 31.5 mol%. As mentioned above, it is more preferably 32 mol% or more, and particularly preferably 33 mol% or more. The hydroxyl group content (hydroxyl group amount) of the polyvinyl acetal resin (1) is preferably 37 mol% or less, more preferably 36.5 mol% or less, still more preferably 36 mol% or less. When the content of the hydroxyl group is at least the above lower limit, the bending rigidity is further increased and the adhesive force of the molded product is further increased. Further, when the content of the hydroxyl group is not more than the above upper limit, the flexibility of the molded body is increased and the handling of the molded body becomes easy.

The hydroxyl group content (hydroxyl group amount) of the polyvinyl acetal resin (1) is preferably 17 mol% or more, more preferably 20 mol% or more, still more preferably 22 mol% or more, preferably 28 mol% or less, more preferably. Is 27 mol% or less, more preferably 25 mol% or less, and particularly preferably 24 mol% or less. When the polyvinyl acetal resin (1) is used as a part of a multilayer molded product, it is particularly preferable to satisfy the lower and upper limits of the hydroxyl group content. When the content of the hydroxyl group is at least the above lower limit, the mechanical strength of the molded product is further increased. In particular, when the content of the hydroxyl group of the polyvinyl acetal resin (1) is 20 mol% or more, the reaction efficiency is high and the productivity is excellent, and when it is 28 mol% or less, the sound insulation of the laminated glass is further improved. .. Further, when the content of the hydroxyl group is not more than the above upper limit, the flexibility of the molded body is increased and the handling of the molded body becomes easy. In particular, laminated glass using a molded body having a hydroxyl group content of 28 mol% or less in the polyvinyl acetal resin (1) tends to have low bending rigidity, but the bending rigidity is remarkably increased by the configuration of the present invention. Can be improved.

The content of each hydroxyl group 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, still more preferably. It is 31.5 mol% or more, more preferably 32 mol% or more, and particularly preferably 33 mol% or more. The hydroxyl group content of the polyvinyl acetal resin (2) and the polyvinyl acetal resin (3) is preferably 37 mol% or less, more preferably 36.5 mol% or less, still more preferably 36 mol% or less. When the content of the hydroxyl group is at least the above lower limit, the bending rigidity is further increased and the adhesive force of the molded product is further increased. Further, when the content of the hydroxyl group is not more than the above upper limit, the flexibility of the molded body is increased and the handling of the molded body becomes easy.

From the viewpoint of further enhancing the sound insulation property, 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 enhancing the sound insulation property, 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). From the viewpoint of further enhancing the sound insulation property, 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 preferably 1 mol% or more. , More preferably 5 mol% or more, still more preferably 9 mol% or more, particularly preferably 10 mol% or more, and most preferably 12 mol% or more. From the viewpoint of further enhancing the sound insulation property, 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 preferably 1 mol% or more. , More preferably 5 mol% or more, still more preferably 9 mol% or more, particularly preferably 10 mol% or more, and most preferably 12 mol% or more. 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 preferably 20 mol% or less. 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 preferably 20 mol% or less.

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

The degree of acetylation (acetyl group amount) of the polyvinyl acetal resin (1) is preferably 0.01 mol% or more, more preferably 0.1 mol% or more, still more preferably 7 mol% or more, still more preferably 9. It is mol% or more, preferably 30 mol% or less, more preferably 25 mol% or less, still more preferably 24 mol% or less. When the degree of acetylation is equal to or higher than the above lower limit, the compatibility between the polyvinyl acetal resin and the plasticizer or other thermoplastic resin becomes high, the sound insulation and penetration resistance are further improved, and the performance over a long period of time is further improved. Stabilize. When the degree of acetylation is not more than the above upper limit, the moisture resistance of the molded product and the laminated glass becomes 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 penetration resistance is further excellent.

The degree of acetylation of the polyvinyl acetal resin (2) and the polyvinyl acetal resin (3) is preferably 0.01 mol% or more, more preferably 0.5 mol% or more, preferably 10 mol% or less, more preferably. Is less than 2 mol%. When the degree of acetylation is at least the above lower limit, the compatibility between the polyvinyl acetal resin and the plasticizer becomes high. When the degree of acetylation is not more than the above upper limit, the moisture resistance of the molded product and the laminated glass becomes high.

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

The degree of acetalization (in the case of polyvinyl butyral resin, the degree of butyralization) of the polyvinyl acetal resin (1) is preferably 47 mol% or more, more preferably 60 mol% or more, still more preferably 68 mol% or more, preferably 68 mol% or more. It is 85 mol% or less, more preferably 80 mol% or less, still more preferably 75 mol% or less. When the degree of acetalization is at least the above lower limit, the compatibility between the polyvinyl acetal resin and the plasticizer becomes high. When the degree of acetalization is not more than the above upper limit, the reaction time required for producing the polyvinyl acetal resin is shortened.

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

The degree of acetalization is determined as follows. First, the value obtained by subtracting the amount of ethylene groups to which the hydroxyl group is bonded and the amount of ethylene groups to which the acetyl group is bonded is obtained from the total amount of ethylene groups in the main chain. The obtained value is divided by the total ethylene group content of the main chain to obtain the mole fraction. The value obtained by expressing this mole fraction as a percentage is the degree of acetalization.

The hydroxyl group content (hydroxyl group amount), acetalization degree (butyralization degree), and acetylation degree are preferably calculated from the results measured by a method based on JIS K 6728 "polyvinyl butyral test method". However, measurement by ASTM D1396-92 may be used. When the polyvinyl acetal resin is a polyvinyl butyral resin, the hydroxyl group content (hydroxyl group amount), the acetalization degree (butyralization degree), and the acetylation degree are based on JIS K6728 "polyvinyl butyral test method". Can be calculated from the results measured by.

(Plasticizer)
The molded product preferably contains a plasticizer. The first layer (including a single-layer molded product) preferably contains a plasticizer (hereinafter, may be referred to as a plasticizer (1)). The second layer preferably contains a plasticizer (hereinafter, may be referred to as a plasticizer (2)). The third layer preferably contains a plasticizer (hereinafter, may be referred to as a plasticizer (3)). By using a plasticizer and by using a polyvinyl acetal resin and a plasticizer in combination, the penetration resistance is further improved, and the adhesive strength of the layer containing the polyvinyl acetal resin and the plasticizer to the laminated glass member or other layers is moderately high. Become. The plasticizer is not particularly limited. The plasticizer (1), the plasticizer (2), and the plasticizer (3) may be the same or different. The plasticizer (1), the plasticizer (2), and the plasticizer (3) may be used alone or in combination of two or more.

Examples of the plasticizer include organic ester plasticizers such as monobasic organic acid esters and polybasic organic acid esters, and organic phosphoric acid plasticizers such as organic phosphoric acid plasticizers and organic subphosphoric acid plasticizers. .. Organic ester plasticizers are preferred. The plasticizer is preferably a liquid plasticizer.

Examples of the monobasic organic acid ester include glycol esters obtained by reacting glycol with a monobasic organic acid. Examples of the glycol include triethylene glycol, tetraethylene glycol, tripropylene glycol and the like. Examples of the monobasic organic acid include butyric acid, isobutyric acid, caproic acid, 2-ethylbutyric acid, heptyl acid, n-octyl acid, 2-ethylhexic acid, n-nonyl acid and decyl acid.

Examples of the polybasic organic acid ester include an ester compound of a polybasic organic acid and an alcohol having a linear or branched structure having 4 to 8 carbon atoms. Examples of the polybasic organic acid include adipic acid, sebacic acid, azelaic acid and the like.

Examples of the organic ester plasticizer include triethylene glycol di-2-ethylpropanoate, triethylene glycol di-2-ethylbutyrate, triethylene glycol di-2-ethylhexanoate, and triethylene glycol dicaprelate. 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, diethylene glycol di-2-ethylbutyrate, diethylene glycol di-2-ethylhexanoate, dipropylene glycol Di-2-ethylbutyrate, triethylene glycol di-2-ethylpentanoate, tetraethylene glycol di-2-ethylbutyrate, diethylene glycol dicaprelate, diethylene glycol dibenzoate, dipropylene glycol dibenzoate, dibutyl maleate, Bis (2-butoxyethyl) adipate, dibutyl adipate, diisobutyl adipate, 2,2-butoxyethoxyethyl adipate, glycol ester benzoate, 1,3-butylene glycol polyester adipate, dihexyl adipate, dioctyl adipate , Hexylcyclohexyl adipate, mixture of heptyl adipate and nonyl adipate, diisononyl adipate, diisodecyl adipate, heptylnonyl adipate, tributyl citrate, tributyl acetylcitrate, diethyl carbonate, dibutyl sebacate, oil-modified alkydic sebacate , And a mixture of a phosphate ester and an adipic acid ester. Organic ester plasticizers other than these may be used. Other adipate esters other than the above-mentioned adipate ester may be used.

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

The plasticizer is preferably a diester plasticizer represented by the following formula (1).

In the above formula (1), 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 of 3 to 10. .. Each of R1 and R2 in the above formula (1) is preferably an organic group having 5 to 10 carbon atoms, and more preferably an organic group having 6 to 10 carbon atoms.

The plasticizer preferably contains triethylene glycol di-2-ethylhexanoate (3GO), triethylene glycol di-2-ethylbutyrate (3GH) or triethylene glycol di-2-ethylpropanoate. .. The plasticizer more preferably contains triethylene glycol di-2-ethylhexanoate or triethylene glycol di-2-ethylbutyrate, and further preferably contains triethylene glycol di-2-ethylhexanoate. preferable.

From the viewpoint of further increasing the breaking elongation and breaking strength at low temperature and high speed, the molded product does not contain a plasticizer, or the polyvinyl acetal resin and the polymer are 100 parts by weight in total. It is preferable that the plasticizer is contained in an amount of 10 parts by weight or less (preferably 5 parts by weight or less). From the viewpoint of further enhancing the penetration resistance, the molded product preferably contains a plasticizer, and 0.01 part by weight or more of the plasticizer is added to 100 parts by weight of the total of the polyvinyl acetal resin and the polymer. It is preferably contained in (preferably 0.1 parts by weight or more).

In the second layer, 100 parts by weight of the thermoplastic resin (2) (100 parts by weight of the polyvinyl acetal resin (2) when the thermoplastic resin (2) is the polyvinyl acetal resin (2)). The content of the agent (2) is defined as the content (2). In the third layer, 100 parts by weight of the thermoplastic resin (3) (100 parts by weight of the polyvinyl acetal resin (3) when the thermoplastic resin (3) is the polyvinyl acetal resin (3)). The content of the agent (3) is defined as the content (3). The content (2) and the content (3) are preferably 10 parts by weight or more, more preferably 15 parts by weight or more, preferably 40 parts by weight or less, more preferably 35 parts by weight or less, still more preferably 32. By weight or less, particularly preferably 30 parts by weight or less. When the content (2) and the content (3) are at least the above lower limit, the flexibility of the molded product is increased and the handling of the molded product becomes easy. When the content (2) and the content (3) are not more than the upper limit, the bending rigidity is further increased.

In the first layer, 100 parts by weight of the thermoplastic resin (1) (100 parts by weight of the polyvinyl acetal resin (1) when the thermoplastic resin (1) is the polyvinyl acetal resin (1)). The content of the agent (1) is defined as the content (1). The content (1) is preferably 1 part by weight or more, more preferably 2 parts by weight or more, still more preferably 3 parts by weight or more, still more preferably 5 parts by weight or more, preferably 90 parts by weight or less, more preferably 90 parts by weight or less. It is 85 parts by weight or less, more preferably 80 parts by weight or less. When the content (1) is at least the above lower limit, the flexibility of the molded product is increased and the handling of the molded product becomes easy. When the content (1) is not more than the upper limit, the penetration resistance of the laminated glass is further increased. The content (1) may be 50 parts by weight or more, 55 parts by weight or more, or 60 parts by weight or more. The content (1) may be 30 parts by weight or less, 20 parts by weight or less, or 10 parts by weight or less.

When the molded product has two or more layers, the content (1) is preferably higher than the content (2) in order to improve the sound insulation of the laminated glass, and the content (1) is It is preferably higher than the above content (3). In particular, laminated glass using a molded body having a content (1) of 55 parts by weight or more tends to have low bending rigidity, but the configuration of the present invention can significantly improve bending rigidity.

From the viewpoint of further improving the sound insulation of the laminated glass, the absolute value of the difference between the above-mentioned content (2) and the above-mentioned content (1), and the difference between the above-mentioned content (3) and the above-mentioned content (1). The absolute value of each is preferably 10 parts by weight or more, more preferably 15 parts by weight or more, still more preferably 20 parts by weight or more. The absolute value of the difference between the content (2) and the content (1) and the absolute value of the difference between the content (3) and the content (1) are preferably 80 parts by weight or less, respectively. It is more preferably 75 parts by weight or less, still more preferably 70 parts by weight or less.

(Heat-shielding substance)
The molded product preferably contains a heat-shielding substance (heat-shielding compound). The first layer preferably contains a heat-shielding substance. The second layer preferably contains a heat-shielding substance. The third layer preferably contains a heat-shielding substance. As the heat-shielding substance, only one kind may be used, or two or more kinds may be used in combination.

The heat-shielding substance preferably contains at least one component X of the phthalocyanine compound, the naphthalocyanine compound and the anthracyanine compound, or preferably contains heat-shielding particles. In this case, both the component X and the heat-shielding particles may be contained.

Ingredient X:
The molded product preferably contains at least one component X of the phthalocyanine compound, the naphthalocyanine compound and the anthracyanine compound. The first layer preferably contains the component X. The second layer preferably contains the component X. The third layer preferably contains the component X. The component X is a heat-shielding substance. As the component X, only one kind may be used, or two or more kinds may be used in combination.

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

From the viewpoint of further improving the heat-shielding property of the molded body and the laminated glass, the component X is preferably at least one selected from the group consisting of phthalocyanine, phthalocyanine derivative, naphthalocyanine and naphthalocyanine derivative. , Phthalocyanine and at least one of the derivatives of phthalocyanine are more preferable.

From the viewpoint of effectively enhancing the heat shielding property and maintaining the visible light transmittance at a higher level for a long period of time, the component X preferably contains a vanadium atom or a copper atom. The component X preferably contains a vanadium atom, and preferably contains a copper atom. The component X is more preferably at least one of a vanadium atom or a copper atom-containing phthalocyanine and a vanadium atom or a copper atom-containing phthalocyanine derivative. From the viewpoint of further improving the heat-shielding property of the molded body and the laminated glass, it is preferable that the component X has a structural unit in which an oxygen atom is bonded to a vanadium atom.

The content of the component X is preferably 0.001% by weight or more, more preferably 0.005 in 100% by weight of the layer containing the component X (first layer, second layer or third layer). By weight% or more, more preferably 0.01% by weight or more, and particularly preferably 0.02% by weight or more. The content of the component X is preferably 0.2% by weight or less, more preferably 0.1 in 100% by weight of the layer containing the component X (first layer, second layer or third layer). It is 0% by weight or less, more preferably 0.05% by weight or less, and particularly preferably 0.04% by weight or less. When the content of the component X is not less than the above lower limit and not more than the above upper limit, the heat shielding property is sufficiently high and the visible light transmittance is sufficiently high. For example, the visible light transmittance can be 70% or more.

Heat shield particles:
The molded product preferably contains heat-shielding particles. The first layer (including a single-layer molded product) preferably contains the heat-shielding particles. The second layer preferably contains the heat shield particles. The third layer preferably contains the heat-shielding particles. The heat-shielding particles are heat-shielding substances. Infrared rays (heat rays) can be effectively blocked by using heat-shielding particles. Only one kind of the heat shield particles may be used, or two or more kinds may be used in combination.

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

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

Specific examples of the heat shield particles include aluminum-doped tin oxide particles, indium-doped tin oxide particles, antimony-doped tin oxide particles (ATO particles), gallium-doped zinc oxide particles (GZO particles), and indium-doped zinc oxide particles (IZO particles). ), Aluminum-doped zinc oxide particles (AZO particles), niob-doped titanium oxide particles, sodium-doped tungsten oxide particles, cesium-doped tungsten oxide particles, tallium-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 other metal oxide particles, hexaborocarbonated lanthanum (LaB ₆ ) particles and the like. Heat-shielding particles other than these may be used. Metal oxide particles are preferable, ATO particles, GZO particles, IZO particles, ITO particles or tungsten oxide particles are more preferable, and ITO particles or tungsten oxide particles are particularly preferable, because the heat ray shielding function is high. In particular, tin-doped indium oxide particles (ITO particles) are preferable, and tungsten oxide particles are also preferable, because they have a high heat ray shielding function and are easily available.

From the viewpoint of further improving the heat-shielding property of the molded product and the laminated glass, the tungsten oxide particles are preferably metal-doped tungsten oxide particles. The above-mentioned "tungsten oxide particles" include metal-doped tungsten oxide particles. Specific examples of the metal-doped tungsten oxide particles include sodium-doped tungsten oxide particles, cesium-doped tungsten oxide particles, thallium-doped tungsten oxide particles, rubidium-doped tungsten oxide particles, and the like.

Cesium-doped tungsten oxide particles are particularly preferable from the viewpoint of further increasing the heat-shielding property of the molded product and the laminated glass. From the viewpoint of further improving the heat-shielding property of the molded body and the laminated glass, the cesium-doped tungsten oxide particles are preferably tungsten oxide particles represented by the _{formula: Cs 0.33} WO _3.

The average particle size 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. When the average particle size is at least the above lower limit, the heat ray shielding property becomes sufficiently high. When the average particle size is not more than the above upper limit, the dispersibility of the heat shield particles becomes high.

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

The content of the heat-shielding particles is preferably 0.01% by weight or more, more preferably 0 in 100% by weight of the layer containing the heat-shielding particles (first layer, second layer or third layer). .1% by weight or more, more preferably 1% by weight or more, and particularly preferably 1.5% by weight or more. The content of the heat-shielding particles is preferably 6% by weight or less, more preferably 5.5 in 100% by weight of the layer containing the heat-shielding particles (first layer, second layer or third layer). It is 0% by weight or less, 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 heat-shielding particles is not less than the above lower limit and not more than the above upper limit, the heat-shielding property is sufficiently high and the visible light transmittance is sufficiently high.

(Metal salt)
The molded body preferably contains at least one metal salt (hereinafter, may be referred to as metal salt M) among an alkali metal salt, an alkaline earth metal salt and a magnesium salt. The first layer preferably contains the metal salt M. The second layer preferably contains the metal salt M. The third layer preferably contains the metal salt M. By using the metal salt M, it becomes easy to control the adhesiveness between the molded body and the laminated glass member or the adhesiveness between each layer in the molded body. As the metal salt M, only one kind may be used, or two or more kinds may be used in combination.

The 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 contained in the molded product preferably contains at least one of K and Mg.

The metal salt M is an alkali metal salt of an organic acid having 2 to 16 carbon atoms, an alkaline earth metal salt of an organic acid having 2 to 16 carbon atoms, or a magnesium salt of an organic acid having 2 to 16 carbon atoms. Is more preferable, and a magnesium carboxylic acid salt having 2 to 16 carbon atoms or a potassium carboxylic acid salt having 2 to 16 carbon atoms is further preferable.

Examples of the magnesium carboxylic acid salt having 2 to 16 carbon atoms and the potassium carboxylic acid salt having 2 to 16 carbon atoms include magnesium acetate, potassium acetate, magnesium propionate, potassium propionate, magnesium 2-ethylbutyrate, and 2-ethylbutanoic acid. Examples thereof include potassium, magnesium 2-ethylhexanoate and potassium 2-ethylhexanoate.

The total content of Mg and K in the layer containing the metal salt M (first layer, second layer or third layer) is preferably 5 ppm or more, more preferably 10 ppm or more, still more preferably 20 ppm or more. It is preferably 300 ppm or less, more preferably 250 ppm or less, still more preferably 200 ppm or less. When the total content of Mg and K is not less than the above lower limit and not more than the above upper limit, the adhesiveness between the molded body and the laminated glass member or the adhesiveness between each layer of the molded body can be controlled more satisfactorily.

(UV shielding agent)
The molded product preferably contains an ultraviolet shielding agent. The first layer preferably contains an ultraviolet shielding agent. The second layer preferably contains an ultraviolet shielding agent. The third layer preferably contains an ultraviolet shielding agent. Due to the use of the ultraviolet shielding agent, the visible light transmittance is less likely to decrease even if the molded product and the laminated glass are used for a long period of time. Only one kind of the above-mentioned ultraviolet shielding agent may be used, or two or more kinds thereof may be used in combination.

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

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

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

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

Examples of the ultraviolet shielding agent containing the metal oxide include zinc oxide, titanium oxide, cerium oxide and the like. Further, the surface of the ultraviolet shielding agent containing the metal oxide may be coated. Examples of the coating material on the surface of the ultraviolet shielding agent containing the metal oxide include insulating metal oxides, hydrolyzable organosilicon compounds, silicone compounds and the like.

Examples of the ultraviolet shielding agent having a benzotriazole structure include 2- (2'-hydroxy-5'-methylphenyl) benzotriazole ("TinuvinP" manufactured by BASF), 2- (2'-hydroxy-3', 5'-di-t-butylphenyl) benzotriazole (BASF "Tinuvin320"), 2- (2'-hydroxy-3'-t-butyl-5-methylphenyl) -5-chlorobenzotriazole (BASF) "Tinuvin 326" manufactured by BASF), 2- (2'-hydroxy-3', 5'-di-amylphenyl) benzotriazole ("Tinuvin 328" manufactured by BASF) and the like. Since the ultraviolet shielding agent is excellent in the ability to absorb ultraviolet rays, the ultraviolet shielding agent is preferably an ultraviolet shielding agent having a benzotriazole structure containing a halogen atom, and may be an ultraviolet shielding agent having a benzotriazole structure containing a chlorine atom. More preferred.

Examples of the ultraviolet shielding agent having a benzophenone structure include octabenzone (“Chimassorb81” manufactured by BASF) and the like.

Examples of the ultraviolet shielding agent having the above triazine structure include "LA-F70" manufactured by ADEKA and 2- (4,6-diphenyl-1,3,5-triazine-2-yl) -5-[(hexyl). Oxy] -phenol (“Tinuvin1577FF” manufactured by BASF) and the like can be mentioned.

Examples of the ultraviolet shielding agent having a malonic acid ester structure include 2- (p-methoxybenzylidene) dimethyl malonate, tetraethyl-2,2- (1,4-phenylenedimethylidene) bismaronate, and 2- (p-methoxybenzylidene). -Bis (1,2,2,6,6-pentamethyl4-piperidinyl) malonate and the like can be mentioned.

Examples of commercially available products of the ultraviolet shielding agent having a malonic acid ester structure include Hostavin B-CAP, Hostavin PR-25, and Hostavin PR-31 (all manufactured by Clariant).

Examples of the ultraviolet shielding agent having an oxalic acid anilides structure include N- (2-ethylphenyl) -N'-(2-ethoxy-5-t-butylphenyl) oxalic acid diamide and N- (2-ethylphenyl)-. A oxalic acid diamide having an aryl group substituted on a nitrogen atom such as N'-(2-ethoxy-phenyl) oxalic acid diamide, 2-ethyl-2'-ethoxy-oxyanilide ("SanduvorVSU" manufactured by Clariant). Kind is mentioned.

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

The content of the ultraviolet shielding agent is preferably 0.1% by weight or more, more preferably 0 in 100% by weight of the layer containing the ultraviolet shielding agent (first layer, second layer or third layer). .2% by weight or more, more preferably 0.3% by weight or more, and particularly preferably 0.5% by weight or more. The content of the ultraviolet shielding agent is preferably 2.5% by weight or less, more preferably 2 in 100% by weight of the layer containing the ultraviolet shielding agent (first layer, second layer or third layer). It is 0% by weight or less, more preferably 1% by weight or less, and particularly preferably 0.8% by weight or less. When the content of the ultraviolet shielding agent is not less than the above lower limit and not more than the above upper limit, it is possible to further suppress the decrease in the visible light transmittance after the lapse of the period. In particular, when the content of the ultraviolet shielding agent is 0.2% by weight or more in 100% by weight of the layer containing the ultraviolet shielding agent, the visible light transmittance of the molded body and the laminated glass after a period of time is lowered. It can be significantly suppressed.

(Antioxidant)
The molded product preferably contains an antioxidant. The first layer preferably contains an antioxidant. The second layer preferably contains an antioxidant. The third layer preferably contains an antioxidant. Only one kind of the above-mentioned antioxidant may be used, or two or more kinds may be used in combination.

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

The above-mentioned antioxidant is preferably a phenol-based antioxidant or a phosphorus-based antioxidant.

Examples of the phenolic antioxidant include 2,6-di-t-butyl-p-cresol (BHT), butyl hydroxyanisole (BHA), 2,6-di-t-butyl-4-ethylphenol, and stearyl-. β- (3,5-di-t-butyl-4-hydroxyphenyl) propionate, 2,2'-methylenebis- (4-methyl-6-butylphenol), 2,2'-methylenebis- (4-ethyl-6) -T-butylphenol), 4,4'-butylidene-bis- (3-methyl-6-t-butylphenol), 1,1,3-tris- (2-methyl-hydroxy-5-t-butylphenyl) butane , Tetrakiss [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) ethylene bis (oxyethylene) and the like. One or more of these antioxidants are preferably used.

Examples of the phosphorus-based antioxidant include tridecylphosphite, tris (tridecyl) phosphite, triphenylphosphite, trinonylphenylphosphite, bis (tridecyl) pentaerythritol diphosphite, and bis (decyl) pentaerythritol diphos. Fight, 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) phosphorous and the like. One or more of these antioxidants are preferably used.

Examples of commercially available products of the above-mentioned antioxidants include "IRGANOX 245" manufactured by BASF, "IRGAFOS 168" manufactured by BASF, "IRGAFOS 38" manufactured by BASF, "Smilizer BHT" manufactured by Sumitomo Chemical Co., Ltd., and "Smilizer BHT" manufactured by Sakai Chemical Industry Co., Ltd. Examples thereof include "H-BHT" and "IRGANOX 1010" manufactured by BASF.

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

(Other ingredients)
The molded product, the first layer, the second layer, and the third layer are each a coupling agent containing silicon, aluminum, or titanium, a dispersant, a surfactant, a flame retardant, as required. It may contain additives such as antistatic agents, fillers, pigments, dyes, adhesive strength modifiers, moisture resistant agents, fluorescent whitening agents and infrared absorbers. Only one of these additives may be used, or two or more of these additives may be used in combination.

In order to control the shear storage modulus to a suitable range, the molded product, the first layer, the second layer and the third layer may contain a filler. Examples of the filler include calcium carbonate particles and silica particles. Silica particles are preferable from the viewpoint of effectively increasing the bending rigidity and effectively suppressing the decrease in transparency.

The content of the filler in 100% by weight of the layer containing the filler (first layer, second layer or third layer) is preferably 1% by weight or more, more preferably 5% by weight or more, still more preferably. It is 10 parts by weight or more, preferably 60% by weight or less, and more preferably 50% by weight or less.

(Other details of the molded product)
The thickness of the molded product is not particularly limited. From the viewpoint of practical use, and from the viewpoint of sufficiently enhancing the penetration resistance and bending rigidity of the laminated glass, the thickness of the molded body is preferably 0.1 mm or more, more preferably 0.25 mm or more, preferably 3 mm or less, and more. It is preferably 1.5 mm or less. When the thickness of the molded body is at least the above lower limit, the penetration resistance and bending rigidity of the laminated glass are further increased. When the thickness of the molded product is not more than the above upper limit, the transparency of the molded product becomes even better.

When the molded product is an interlayer film, the thickness of the interlayer film is T. The thickness of the first layer is preferably 0.035 T or more, more preferably 0.0625 T or more, still more preferably 0.1 T or more, preferably 0.4 T or less, still more preferably 0.375 T or less, still more preferably. It is 0.25T or less, particularly preferably 0.15T or less. When the thickness of the first layer is 0.4 T or less, the bending rigidity becomes even better.

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

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

The interlayer film may be an interlayer film having a uniform thickness or an interlayer film having a variable thickness. The cross-sectional shape of the interlayer film may be rectangular or wedge-shaped.

The method for producing the molded product according to the present invention is not particularly limited. Examples of the method for producing a molded product according to the present invention include a method of extruding a resin composition using an extruder in the case of a single-layer molded product. As a method for producing a molded product according to the present invention, in the case of a multi-layered molded product, for example, each layer is formed by using each resin composition for forming each layer, and then the obtained layers are laminated. , And a method of laminating each layer by co-extruding each resin composition for forming each layer using an extruder. Since it is suitable for continuous production, a manufacturing method of extrusion molding is preferable.

Since the production efficiency of the molded product is excellent, it is preferable that the second layer and the third layer contain the same polyvinyl acetal resin. Since the production efficiency of the interlayer film is excellent, it is more preferable that the second layer and the third layer contain the same polyvinyl acetal resin and the same plasticizer. It is more preferable that the second layer and the third layer are formed of the same resin composition because the intermediate film production efficiency is excellent.

The molded product preferably has an uneven shape on at least one of the surfaces on both sides. It is more preferable that the molded product has an uneven shape on both surfaces. The method for forming the uneven shape is not particularly limited, and examples thereof include a lip embossing method, an embossing roll method, a calendar roll method, and a deformed extrusion method. The embossing roll method is preferable because it is possible to form embossing of a large number of uneven shapes which are quantitatively constant uneven patterns.

(Laminated glass)
FIG. 3 is a cross-sectional view schematically showing an example of a laminated glass using the interlayer film for laminated glass shown in FIG.

The laminated glass 31 shown in FIG. 3 includes a first laminated glass member 21, a second laminated glass member 22, and an interlayer film 11. The interlayer film 11 is arranged between the first laminated glass member 21 and the second laminated glass member 22 and is sandwiched therein.

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

FIG. 4 is a cross-sectional view schematically showing an example of a laminated glass using the laminated glass interlayer film shown in FIG. 2.

The laminated glass 31A shown in FIG. 4 includes a first laminated glass member 21, a second laminated glass member 22, and an interlayer film 11A. The interlayer film 11A is arranged between the first laminated glass member 21 and the second laminated glass member 22 and is sandwiched therein.

The first laminated glass member 21 is laminated on the first surface 11a of the interlayer film 11A. The second laminated glass member 22 is laminated on the second surface 11b opposite to the first surface 11a of the interlayer film 11A.

As described above, the laminated glass according to the present invention includes a first laminated glass member, a second laminated glass member, and a molded body (intermediate film), and the molded body (intermediate film) is the present invention. It is a molded body according to the invention. In the laminated glass according to the present invention, the molded body is arranged between the first laminated glass member and the second laminated glass member.

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

Examples of the laminated glass member include a glass plate and a PET (polyethylene terephthalate) film. The laminated glass includes not only laminated glass in which a molded body is sandwiched between two glass plates, but also laminated glass in which a molded body is sandwiched between a glass plate and a PET film or the like. The laminated glass is a laminated body provided with a glass plate, and it is preferable that at least one glass plate is used. The first laminated glass member and the second laminated glass member are glass plates or PET films, respectively, and the laminated glass is the first laminated glass member and the second laminated glass member. It is preferable to provide a glass plate as at least one of them.

Examples of the glass plate include inorganic glass and organic glass. Examples of the inorganic glass include float plate glass, heat ray absorbing plate glass, heat ray reflecting plate glass, polished plate glass, template glass, and wire-filled plate glass. The organic glass is a synthetic resin glass that replaces the inorganic glass. Examples of the organic glass include a polycarbonate plate and a poly (meth) acrylic resin plate. Examples of the poly (meth) acrylic resin plate include a polymethyl (meth) acrylate plate.

The thickness of the laminated glass member is preferably 1 mm or more, preferably 5 mm or less, and more preferably 3 mm or less. When 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. When the laminated glass member is a PET film, the thickness of the PET film is preferably 0.03 mm or more, preferably 0.5 mm or less.

By using the molded body according to the present invention, the bending rigidity of the laminated glass can be maintained high even if the thickness of the laminated glass is thin. The thickness of the glass plate is preferably 2 mm or less, more preferably 1.8 mm or less, still more preferably 1.6 mm or less, still more preferably 1.5 mm or less, still more preferably 1.4 mm or less, still more preferably 1. It is 0.3 mm or less, more preferably 1.0 mm or less, and particularly preferably 0.7 mm or less. In this case, it is possible to reduce the weight of the laminated glass, reduce the material of the laminated glass to reduce the environmental load, and improve the fuel efficiency of the automobile by reducing the weight of the laminated glass to reduce the environmental load. .. The total of the thickness of the first glass plate and the thickness of the second glass plate is preferably 3.5 mm or less, more preferably 3.2 mm or less, still more preferably 3 mm or less, and particularly preferably 2.8 mm or less. Is. In this case, it is possible to reduce the weight of the laminated glass, reduce the material of the laminated glass to reduce the environmental load, and improve the fuel efficiency of the automobile by reducing the weight of the laminated glass to reduce the environmental load. ..

The method for producing the laminated glass is not particularly limited. First, a molded body is sandwiched between the first laminated glass member and the second laminated glass member to obtain a laminated body. Next, for example, by passing the obtained laminated body through a pressing roll or putting it in a rubber bag and sucking it under reduced pressure, the first laminated glass member, the second laminated glass member, and the molded body are combined. Degas the air remaining in between. Then, it is pre-bonded at about 70 to 110 ° C. to obtain a pre-bonded laminate. Next, the pre-crimped laminate is placed in an autoclave or pressed, and crimped at a pressure of about 120 to 150 ° C. and 1 to 1.5 MPa. In this way, laminated glass can be obtained. At the time of manufacturing the laminated glass, the first layer, the second layer and the third layer may be laminated.

The molded body and the laminated glass can be used for automobiles, railroad vehicles, aircraft, ships, buildings and the like. The molded body and the laminated glass can be used for other purposes. The molded body and the laminated glass are preferably a molded body and a laminated glass for a vehicle or a building, and more preferably an interlayer film and a laminated glass for a vehicle. The molded body and the laminated glass can be used for the windshield, side glass, rear glass, roof glass and the like of an automobile. The molded body and the laminated glass are preferably used for automobiles. The molded body is used to obtain laminated glass for automobiles.

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

The following materials were prepared.

(Polyvinyl acetal resin)
The polyvinyl acetal resins shown in Tables 1 to 3 below were appropriately used.

For the polyvinyl acetal resin, the degree of acetalization, the degree of acetylation and the content of hydroxyl groups were measured by a method according to JIS K6728 "Polyvinyl butyral test method". In addition, when measured by ASTM D1396-92, the same numerical value as the method based on JIS K6728 "polyvinyl butyral test method" was shown. When the type of acetal is acet acetal, benzyl acetal or cumin acetal, the degree of acetalization is similarly measured by measuring the degree of acetylation and the content of hydroxyl groups, and the molar fraction is calculated from the obtained measurement results. It is calculated and then calculated by subtracting the degree of acetylation and the content of hydroxyl groups from 100 mol%.

(Second resin)
The acrylic polymers shown in Tables 1 to 3 below were appropriately used.

The acrylic polymer shown in Tables 1 to 3 below is an acrylic polymer obtained by polymerizing a polymerizable component containing the following compounds at the contents shown in Tables 1 to 3 below.

Ethyl Acrylic Acid Butyl Acrylic Acid Benzyl Acrylic Acid 2-Hydroxyethyl Acrylic Acid Glycyl Methacrylic Acid Tripropylene Glycoldiacrylate (“APG-200” manufactured by Shin-Nakamura Chemical Co., Ltd.)
Polypropylene glycol # 400 diacrylate ("APG-400" manufactured by Shin-Nakamura Chemical Co., Ltd.)
Polypropylene glycol (# 700) diacrylate ("APG-700" manufactured by Shin-Nakamura Chemical Co., Ltd.)
Ethoxylated bisphenol A diacrylate ("A-BPE-20" manufactured by Shin-Nakamura Chemical Co., Ltd.)
ε-Caprolactone-modified tris- (2-acryloxyethyl) isocyanurate ("A-9300-1CL" manufactured by Shin-Nakamura Chemical Co., Ltd.)
Tris Phosphate [2- (Acryloyloxy) Ethyl]
Ethoxylated pentaerythritol tetraacrylate ("ATM-35E" manufactured by Shin-Nakamura Chemical Co., Ltd.)

(Plasticizer)
Triethylene glycol di-2-ethylhexanoate (3GO)

(Example 1)
A polyvinyl acetal resin (average degree of polymerization 560, acetalization degree 74.0 mol%, hydroxyl group content 25.0 mol%, acetylation degree 0.9 mol%) was prepared. 100 parts by weight of the polymerizable component (60 parts by weight of ethyl acrylate, 14.2 parts by weight of butyl acrylate, 25.2 parts by weight of benzyl acrylate, 0.6 parts by weight of tripropylene glycol diacrylate) was prepared. In a reaction vessel equipped with a thermometer, a stirrer, a nitrogen introduction tube, and a cooling tube, 100 parts by weight of the polyvinyl acetal resin as a raw material, 100 parts by weight of the polymerizable component, and 300 parts by weight of ethyl acetate as a polymerization solvent are placed. In addition, the polyvinyl acetal resin was dissolved with stirring. Next, nitrogen gas was blown into the reaction vessel for 30 minutes to replace the inside of the reaction vessel with nitrogen, and then the inside of the reaction vessel was heated to 80 ° C. with stirring. After 30 minutes, 0.5 part by weight of t-butylperoxy-2-ethylhexanoate (1 hour half-life temperature: 92.1 ° C., 10 hour half-life temperature: 72.1 ° C.) as a polymerization initiator was added. The polymerization initiator solution obtained by diluting with 5 parts by weight of ethyl acetate was added dropwise into the reaction vessel over 6 hours. Then, the reaction was further carried out at 80 ° C. for 6 hours, and then the reaction solution was cooled to obtain a solution containing a modified polyvinyl acetal resin.

To the obtained solution, add 5 parts by weight of 3GO as a plasticizer to a total of 100 parts by weight of the polyvinyl acetal resin and the polymer (second resin), and add a diluting solvent (mixed solvent of methanol and toluene, methanol and toluene). The weight ratio was 1: 2) to obtain a solution having a solid content of 20% by weight. Next, this solution was applied to a PET film that had been mold-released to a thickness of 50 μm after drying using a coater, and dried at 80 ° C. for 1 hour to obtain an interlayer film. The obtained interlayer films having a thickness of 50 μm were superposed and heat-bonded at 150 ° C. and 20 MPa to obtain an interlayer film having a thickness of 400 μm.

(Examples 2 to 20 and Comparative Examples 1 to 9)
An interlayer film and a laminated glass were obtained in the same manner as in Example 1 except that the composition of the composition for forming the interlayer film was set as shown in Tables 1 to 3 below.

(evaluation)
(1) Gel fraction 0.2 g of the interlayer film was immersed in 40 g of tetrahydrofuran and shaken and immersed at 23 ° C. for 24 hours. Then, a centrifuge (KUBOTA, high-speed, large-capacity cooling centrifuge 7780) was used to centrifuge at 10 ° C. and 10000 rpm, and then the supernatant was removed. The residue in the container was heated at 110 ° C. for 1 hour to dry. The weight of the residue was then weighed. The gel fraction was calculated by the above formula (X).

(2) Observation of phase structure The obtained interlayer film was treated with a microtome to prepare a section having a thickness of 100 nm. The obtained sections were stained with osmium tetroxide and observed with a transmission electron microscope. The presence or absence of a phase-separated structure was determined.

[Criteria for determining the presence or absence of a phase-separated structure]
◯: With phase separation structure ×: Without phase separation structure

Further, when there is a phase-separated structure and there is a matrix, it was confirmed whether the resin component constituting the matrix and the island (domain) is a polyvinyl acetal resin or a second resin.

[Criteria for determining resin components constituting the matrix and islands]
A: The component constituting the matrix is a polyvinyl acetal resin and the component constituting the island portion is the second resin. B: The component constituting the matrix is the second resin and the component constituting the island portion is the polyvinyl acetal resin.

Further, when there was a phase-separated structure and there was an island portion (domain), the diameter (maximum diameter) of the island portion was observed at 3000 times or 5000 times, and the average value was obtained. The average diameter of the islands was determined according to the following criteria.

[Criteria for averaging island diameters]
A: The average diameter of the islands is 10 nm or more and 1 μm or less. B: Does not correspond to the standard of A.

(3) Tensile characteristics An interlayer film (thickness 400 μm) cut into 5 cm × 1 cm was prepared. The breaking elongation and breaking strength (maximum stress) of the interlayer film were measured with a tensile tester at a low temperature of −20 ° C. and a high speed of 500 mm / min. The tensile elongation and breaking strength were evaluated according to the following criteria.

[Criteria for determining elongation at break]
○ ○: Tensile elongation is 180% or more ○: Tensile elongation is 150% or more and less than 180% Δ: Tensile elongation is 110% or more and less than 150% ×: Tensile elongation is less than 110%

[Breaking strength (criteria for determining maximum stress]
○ ○: Breaking strength is 40 MPa or more ○: Breaking strength is 30 MPa or more and less than 40 MPa Δ: Breaking strength is 20 MPa or more and less than 30 MPa ×: Breaking strength is less than 20 MPa

Details and results are shown in Tables 1 to 3 below.

1 ... 1st layer 1a ... 1st surface 1b ... 2nd surface 2 ... 2nd layer 2a ... outer surface 3 ... 3rd layer 3a ... outer surface 11 ... intermediate film 11A ... intermediate film (first) 1 layer)
11a ... 1st surface 11b ... 2nd surface 21 ... 1st laminated glass member 22 ... 2nd laminated glass member 31 ... laminated glass 31A ... laminated glass

Claims (13)

It contains a polyvinyl acetal resin and a polymer of a polymerizable component containing a (meth) acrylate compound having two or more (meth) acryloyl groups.
The content of the polymer is 85 parts by weight or more and 180 parts by weight or less with respect to 100 parts by weight of the polyvinyl acetal resin.
Have a phase separation structure,
A (meth) acrylate compound having two or more (meth) acryloyl groups and a (meth) acrylate compound having two or more (meth) acryloyl groups in 100% by weight of the polymerizable component constituting the polymer. ) The total amount with the polymerizable compound having an acryloyl group is 50% by weight or more, and the amount is 50% by weight or more.
A molded product in which the polymer is an acrylic polymer. The molded product according to claim 1, which contains no plasticizer or contains 10 parts by weight or less of the plasticizer with respect to 100 parts by weight of the total of the polyvinyl acetal resin and the polymer. The molded product according to claim 1, which contains no plasticizer or contains 5 parts by weight or less of the plasticizer with respect to 100 parts by weight of the total of the polyvinyl acetal resin and the polymer. The molded product according to any one of claims 1 to 3 , which contains a plasticizer. The molded product according to any one of claims 1 to 4 , wherein the gel fraction obtained by the following formula (X) is 0% by weight or more and 50% by weight or less.
Gel fraction (% by weight) = W2 / W1 × 100 ・ ・ ・ Equation (X)
W1: Weight of the molded product before immersing the molded product in tetrahydrofuran at 23 ° C. W2: Weight of the molded product after immersing the molded product in tetrahydrofuran at 23 ° C. and then taking it out and drying it. The molded product according to any one of claims 1 to 5 , wherein the polyvinyl acetal resin and the polymer are crosslinked. The molded product according to any one of claims 1 to 6 , which is an interlayer film for laminated glass. The molded product according to any one of claims 1 to 7 , wherein the thickness is 3 mm or less. Claims 1 to 2, wherein a first glass plate having a thickness of 1.6 mm or less is arranged between the first glass plate and the second glass plate and used to obtain a laminated glass. Item 8. The molded product according to any one of 8. It is placed between the first glass plate and the second glass plate and used to obtain laminated glass.
The molded product according to any one of claims 1 to 9 , wherein the total of the thickness of the first glass plate and the thickness of the second glass plate is 3.5 mm or less. The first laminated glass member and
With the second laminated glass member,
The molded product according to any one of claims 1 to 10 is provided.
A laminated glass in which the molded body is arranged between the first laminated glass member and the second laminated glass member. The first laminated glass member is a first glass plate, and the first laminated glass member is a first glass plate.
The laminated glass according to claim 11 , wherein the thickness of the first glass plate is 1.6 mm or less. The first laminated glass member is a first glass plate, and the first laminated glass member is a first glass plate.
The second laminated glass member is a second glass plate.
The laminated glass according to claim 11 or 12 , wherein the total of the thickness of the first glass plate and the thickness of the second glass plate is 3.5 mm or less.

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