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WO2018181755A1 - Corps moulé et verre feuilleté - Google Patents

Corps moulé et verre feuilleté Download PDF

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Publication number
WO2018181755A1
WO2018181755A1 PCT/JP2018/013336 JP2018013336W WO2018181755A1 WO 2018181755 A1 WO2018181755 A1 WO 2018181755A1 JP 2018013336 W JP2018013336 W JP 2018013336W WO 2018181755 A1 WO2018181755 A1 WO 2018181755A1
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WO
WIPO (PCT)
Prior art keywords
weight
laminated glass
less
layer
meth
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Ceased
Application number
PCT/JP2018/013336
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English (en)
Japanese (ja)
Inventor
晋治 河田
郁 進藤
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Sekisui Chemical Co Ltd
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Sekisui Chemical Co Ltd
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Filing date
Publication date
Application filed by Sekisui Chemical Co Ltd filed Critical Sekisui Chemical Co Ltd
Priority to JP2018519981A priority Critical patent/JP6985259B2/ja
Publication of WO2018181755A1 publication Critical patent/WO2018181755A1/fr
Anticipated expiration legal-status Critical
Ceased legal-status Critical Current

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    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B17/00—Layered products essentially comprising sheet glass, or glass, slag, or like fibres
    • B32B17/06—Layered products essentially comprising sheet glass, or glass, slag, or like fibres comprising glass as the main or only constituent of a layer, next to another layer of a specific material
    • B32B17/10—Layered products essentially comprising sheet glass, or glass, slag, or like fibres comprising glass as the main or only constituent of a layer, next to another layer of a specific material of synthetic resin
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08K—Use of inorganic or non-macromolecular organic substances as compounding ingredients
    • C08K5/00—Use of organic ingredients
    • C08K5/04—Oxygen-containing compounds
    • C08K5/10—Esters; Ether-esters
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
    • C08L29/00—Compositions of homopolymers or copolymers of compounds having one or more unsaturated aliphatic radicals, each having only one carbon-to-carbon double bond, and at least one being terminated by an alcohol, ether, aldehydo, ketonic, acetal or ketal radical; Compositions of hydrolysed polymers of esters of unsaturated alcohols with saturated carboxylic acids; Compositions of derivatives of such polymers
    • C08L29/14—Homopolymers or copolymers of acetals or ketals obtained by polymerisation of unsaturated acetals or ketals or by after-treatment of polymers of unsaturated alcohols
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
    • C08L33/00—Compositions of homopolymers or copolymers of compounds having one or more unsaturated aliphatic radicals, each having only one carbon-to-carbon double bond, and only one being terminated by only one carboxyl radical, or of salts, anhydrides, esters, amides, imides or nitriles thereof; Compositions of derivatives of such polymers
    • C08L33/04—Homopolymers or copolymers of esters
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B60—VEHICLES IN GENERAL
    • B60J—WINDOWS, WINDSCREENS, NON-FIXED ROOFS, DOORS, OR SIMILAR DEVICES FOR VEHICLES; REMOVABLE EXTERNAL PROTECTIVE COVERINGS SPECIALLY ADAPTED FOR VEHICLES
    • B60J1/00—Windows; Windscreens; Accessories therefor

Definitions

  • the present invention relates to a molded article that can be suitably used for an interlayer film for laminated glass and the like. Moreover, this invention relates to the laminated glass using the said molded object.
  • Polyvinyl acetal resin is used for various purposes in laminated glass interlayer films for laminated glass, metal-treated wash primers, various paints, adhesives, resin processing agents, ceramic binders, and the like. In recent years, the use of polyvinyl acetal resin has been expanded to electronic materials and the like.
  • the above laminated glass is excellent in safety because the amount of glass fragments scattered is small even if it is damaged by an external impact. For this reason, the said laminated glass is widely used for a motor vehicle, a rail vehicle, an aircraft, a ship, a building, etc.
  • the laminated glass is manufactured by sandwiching an interlayer film for laminated glass between two glass plates.
  • Patent Document 1 discloses a polyvinyl acetal resin composition containing a polyvinyl acetal resin and a resin having a crosslinked structure.
  • the composition has a structure in which the resin having the crosslinked structure is dispersed as a dispersed phase in the polyvinyl acetal resin as a continuous phase.
  • the composition had a loss tangent maximum value derived from the polyvinyl acetal resin at 40 ° C. or higher and a loss derived from the resin having the crosslinked structure.
  • the maximum value of tangent is 10 ° C. or lower.
  • the resin having the crosslinked structure is a (meth) acrylic resin having a crosslinked structure.
  • Patent Document 2 discloses an intermediate 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 disposed between glass plates having a thickness of 4.0 mm or less.
  • Patent Document 1 describes that excellent mechanical strength is expressed 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.
  • a tensile test is performed at a relatively low speed of 100 mm / min.
  • laminated glass used in automobiles is subjected to deformation stress at a considerably high speed during external impact.
  • a laminated glass may be exposed to a low temperature environment.
  • the inventors of the present invention focused on the problem of further improving the fracture strength against high-speed deformation stress at a low temperature in a molded body such as an intermediate film.
  • a polyvinyl acetal resin and a polymer of a polymerizable component containing a (meth) acrylate compound having two or more (meth) acryloyl groups and 100 parts by weight of the polyvinyl acetal resin
  • a molded product having a content of the polymer of 85 parts by weight or more and 180 parts by weight or less and having a phase separation structure.
  • a (meth) acrylate compound having two or more (meth) acryloyl groups in 100% by weight of the polymerizable component constituting the polymer, a (meth) acrylate compound having two or more (meth) acryloyl groups, and a (meth) acryloyl group.
  • the total amount of the polymerizable compound having a (meth) acryloyl group other than the (meth) acrylate compound having two or more is 50% by weight or more, and the polymer is an acrylic polymer.
  • a molded object does not contain a plasticizer, or 10 parts weight or less of plasticizers with respect to a total of 100 weight part of the said polyvinyl acetal resin and the said polymer. Including.
  • a molded object does not contain a plasticizer, or 5 weight part or less of plasticizers with respect to a total of 100 weight part of the said polyvinyl acetal resin and the said polymer. Including.
  • the molded body includes a plasticizer.
  • the gel fraction obtained by the following formula (X) is 0% by weight or more and 50% by weight or less.
  • the polyvinyl acetal resin and the polymer are crosslinked.
  • the molded body is an interlayer film for laminated glass.
  • the thickness is 3 mm or less.
  • a molded object uses the 1st glass plate which is 1.6 mm or less in thickness, Between the said 1st glass plate and a 2nd glass plate. Arranged and used to obtain laminated glass.
  • a molded object is arrange
  • the total of the thickness of the plate and the thickness of the second glass plate is 3.5 mm or less.
  • the first laminated glass member, the second laminated glass member, and the molded body described above are provided, and the first laminated glass member and the second laminated glass member There is provided a laminated glass in which the molded body is disposed.
  • the first laminated glass member is a first glass plate, and the thickness of the first glass plate is 1.6 mm or less.
  • a said 1st laminated glass member is a 1st glass plate
  • a said 2nd laminated glass member is a 2nd glass plate
  • the said 1st 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 body according to the present invention includes a polyvinyl acetal resin and a polymer of a polymerizable component including 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.
  • the molded body according to the present invention has a phase separation structure. Since the molded body according to the present invention has the above-described configuration, the fracture elongation of the molded body according to the present invention at low temperature and high speed can be increased, and the fracture strength at low temperature and high speed can be increased. it 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 the second embodiment of the present invention.
  • FIG. 3 is a cross-sectional view schematically showing an example of a laminated glass using the laminated glass interlayer film 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.
  • the molded body 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 sometimes 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.
  • the polymer X is used as the second resin other than the polyvinyl acetal resin.
  • 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 body according to the present invention has a phase separation structure.
  • the fracture elongation of the molded body according to the present invention at low temperature and high speed can be increased, and the fracture strength at low temperature and high speed can be increased. it can.
  • the breaking elongation and breaking strength at ⁇ 20 ° C. of the molded product according to the present invention can be increased.
  • the breaking elongation and breaking strength at a high speed of 500 mm / min of the molded body according to the present invention can be increased.
  • the molded body when a molded body is used as the interlayer film for laminated glass, the molded body is often disposed between the first glass plate and the 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 allows the molded body to have a low temperature and high speed elongation at break and a low temperature and high speed breaking strength of the molded body. It is possible to effectively suppress breakage of the glass and scattering of the glass plate. Moreover, even if the thickness of both the 1st glass plate and the 2nd glass plate is thin, damage of a laminated glass and scattering of a glass plate can fully be suppressed by use of the molded object which concerns on this invention. In addition, when both the thickness of the 1st glass plate and the 2nd glass plate is thick, the failure
  • 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 increasing 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. Or less.
  • the molded body has a phase separation structure.
  • the polymer X is preferably an island (domain) in the phase separation structure.
  • One factor for achieving the above effect in the present invention is considered to be that energy distribution proceeds smoothly by the phase separation structure.
  • the polyvinyl acetal resin preferably surrounds the domain, and the polyvinyl acetal resin is preferably a matrix.
  • the phase separation structure is preferably a co-continuous structure or a sea-island structure.
  • the phase separation structure may be a co-continuous structure or a sea-island structure.
  • the polyvinyl acetal resin and the polymer X are preferably contained in different phases.
  • a phase separation structure is preferably formed by the polyvinyl acetal resin and the polymer X.
  • the polyvinyl acetal resin may be a sea part, and the polymer X may be an island part, the polymer X may be a sea part, and the polyvinyl acetal resin may be an island part.
  • 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.
  • the polyvinyl acetal resin may be present in a network form, and the polymer X may be present in a network form.
  • the polyvinyl acetal resin and the polymer X preferably have a sea-island structure or a bicontinuous structure. That is, in the phase separation structure, it is preferable that the polyvinyl acetal resin and the polymer X form a sea-island structure or a bicontinuous 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 ⁇ m or less, more preferably 10 ⁇ m or less, still more preferably. Is 2 ⁇ m or less, particularly preferably 1 ⁇ m or less.
  • the diameter of one island part indicates the maximum diameter, and the average of the island parts is obtained by averaging the diameters (maximum diameters) of a plurality of islands.
  • the gel fraction obtained by the following formula (X) is preferably 0% by weight or more, preferably 50% by weight or less, More preferably, it is 30% by weight or less.
  • the molded body according to the present invention is suitably used as an interlayer film for laminated glass (hereinafter sometimes referred to as an interlayer film).
  • the intermediate film has a single-layer structure or a two-layer structure.
  • the intermediate film may have a single layer structure or a two or more layer structure.
  • the intermediate film may have a two-layer structure or may have a three-layer structure or more.
  • the intermediate film includes a first layer.
  • the intermediate film may be a single-layer intermediate film including only the first layer, or may be a multilayer intermediate film including the first layer and another layer.
  • the intermediate film may have a structure of two or more layers, and may include a second layer in addition to the first layer.
  • the intermediate film preferably further includes a second layer.
  • the second layer is disposed on the first surface side of the first layer.
  • the intermediate 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.
  • the intermediate film preferably further includes a third layer.
  • the third layer is disposed on the second surface side of the first layer opposite to the first surface.
  • 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.
  • stacked on the said 2nd layer becomes like this.
  • it is 1.6 mm or less, More preferably, it is 1.3 mm or less.
  • the second surface opposite to the first surface of the first layer may be a surface on which a laminated glass member or a glass plate is laminated.
  • stacked on the said 1st layer becomes like this.
  • 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 intermediate film is disposed between the first glass plate and the second glass plate and is preferably used for obtaining laminated glass. Since the bending 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 said intermediate film is arrange
  • the intermediate film includes 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 used between the first glass plate and the second glass plate and is more preferably used to obtain laminated glass. Also in this case, the bending rigidity, breaking elongation and breaking strength can be sufficiently increased due to the intermediate film.
  • 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 intermediate film 11 shown in FIG. 1 is a multilayer intermediate film having a structure of two or more layers.
  • the intermediate film 11 is used to obtain a laminated glass.
  • the intermediate film 11 is an intermediate film for laminated glass.
  • the intermediate film 11 includes a first layer 1, a second layer 2, and a third layer 3.
  • On the first surface 1a of the first layer 1, the second layer 2 is disposed and laminated.
  • the third layer 3 is disposed on the second surface 1b opposite to the first surface 1a of the first layer 1 and laminated.
  • the first layer 1 is an intermediate layer.
  • Each of the second layer 2 and the third layer 3 is a protective layer, and is a surface layer in the present embodiment.
  • the first layer 1 is arranged between the second layer 2 and the third layer 3 and is sandwiched between them. Therefore, the intermediate film 11 has a multilayer structure (second layer 2 / first layer 1 / third layer) in which the second layer 2, the first layer 1, and the third layer 3 are laminated in this order. Having layer
  • layers may be disposed between the second layer 2 and the first layer 1 and between the first layer 1 and the third layer 3, respectively.
  • the second layer 2 and the first layer 1 and the first layer 1 and the third layer 3 are preferably laminated directly.
  • examples of other layers include layers 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 the second embodiment of the present invention.
  • the intermediate film 11A shown in FIG. 2 is a single-layer intermediate film having a single-layer structure.
  • the intermediate film 11A is a first layer.
  • the intermediate film 11A is used to obtain a laminated glass.
  • the intermediate film 11A is an intermediate film for laminated glass.
  • the molded body contains a polyvinyl acetal resin and a polymer X of a polymerizable component containing a (meth) acrylate compound having two or more (meth) acryloyl groups.
  • Each of the first layer, the second layer, and the third layer preferably includes a polyvinyl acetal resin.
  • the first layer, the second layer, and the third layer each preferably include the polymer X.
  • the said polyvinyl acetal resin only 1 type may be used and 2 or more types may be used together.
  • the said polymer X only 1 type may be used and 2 or more types may be used together.
  • the polyvinyl acetal resin is a polyvinyl acetoacetal resin, a polyvinyl butyral resin, a polyvinyl benzyl acetal resin, or a polyvinyl cumin acetal.
  • a resin is preferred.
  • the polyvinyl acetal resin is preferably a polyvinyl acetoacetal resin.
  • polyvinyl acetal resins include acetoacetalized resins, benzyl acetalized resins, and cumin acetalized resins.
  • the molded product is a polyolefin resin, an acrylic polymer, a urethane polymer, a silicone polymer, rubber, or vinyl acetate heavy as the polymer X. It is preferable to include a coalescence, and it is more preferable to include 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.
  • the total amount A together with the polymerizable compound having a (meth) acryloyl group is defined as a total amount A.
  • 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, particularly preferably. 80% by weight or more, most preferably 90% 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).
  • (Meth) acrylate compounds pentaerythritol tri (meth) acrylate, trimethylolpropane tri (meth) acrylate, trimethylolethane tri (meth) acrylate di (meth) acrylate, dipentaerythritol tri (meth) acrylate, ⁇ -caprolactone modified tris
  • a trifunctional (meth) acrylate compound such as (2- (meth) acryloxyethyl) isocyanurate, tris [2-((meth) acryloyloxy) ethyl] phosphate; pen 4 or more functional groups such as taerythritol tetra (meth) acrylate, dipentaerythritol tetra (meth) acrylate, ethoxylated pentaerythritol tetra (meth) acrylate, dipentaerythritol penta (meth) acrylate, dipenta
  • 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 poly (meth) acrylate methyl, poly (meth) ethyl acrylate, poly (meth) acrylate n-propyl, poly (meth) acrylate i-propyl, 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, Poly (meth) acrylate 2-hydroxypropyl, poly (meth) acrylate 4-hydroxybutyl, poly (meth) acrylate glycidyl, poly (meth) acrylate octyl, poly (meth) acrylate propyl, poly (meth) 2-ethyloctyl acrylate, poly (meth)
  • Examples of (meth) acrylic acid having a polar group and (meth) acrylic acid ester include (meth) acrylic acid, 2-hydroxyethyl (meth) acrylate, 4-hydroxybutyl (meth) acrylate, and Examples include glycidyl (meth) acrylate.
  • polyacrylate is preferred, and polyethyl acrylate, poly (n-butyl acrylate), poly (acrylic acid) are preferred. 2-ethylhexyl acid or octyl polyacrylate is more preferred.
  • the productivity of the molded body and the balance of the characteristics of the molded body are further improved.
  • the said poly (meth) acrylic acid ester only 1 type may be used and 2 or more types may be used together.
  • the polyvinyl acetal resin and the polymer X are cross-linked.
  • the said molded object may contain the said polyvinyl acetal resin and the said polymer X as a crosslinked material which the said polyvinyl acetal resin and the said polymer X bridge
  • the thermoplastic resin may have a crosslinked structure. With the cross-linked structure, the shear storage elastic modulus can be controlled, and a molded article having both excellent flexibility and high strength can be produced.
  • a method in which crosslinks are formed by introducing functional groups that react with each other into the polymer structure of the resin A method of crosslinking using a crosslinking agent having two or more functional groups that react with a functional group present in the polymer structure of the resin.
  • a method of crosslinking a polymer by using a radical generator having a hydrogen abstraction ability such as peroxide A method of crosslinking by electron beam irradiation. Since it is easy to control the shear storage elastic modulus and the productivity of the molded body is high, a method of forming crosslinks by introducing functional groups that react with each other into the polymer structure of the resin is preferable.
  • 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 a step of forming a polymer X by polymerization to obtain a molded body is performed. By this step, a structure in which the polyvinyl acetal resin and the polymer X are cross-linked is formed.
  • the first layer (including a single-layer molded body) preferably contains a thermoplastic resin (hereinafter sometimes referred to as a thermoplastic resin (1)).
  • the first layer preferably contains a polyvinyl acetal resin (hereinafter sometimes referred to as a polyvinyl acetal resin (1)) as the thermoplastic resin (1).
  • the molded body contains the polyvinyl acetal resin (1).
  • the second layer preferably contains a thermoplastic resin (hereinafter sometimes referred to as a thermoplastic resin (2)).
  • the second layer preferably contains a polyvinyl acetal resin (hereinafter sometimes referred to as a polyvinyl acetal resin (2)) as the thermoplastic resin (2).
  • the third layer preferably contains a thermoplastic resin (hereinafter sometimes referred to as a thermoplastic resin (3)).
  • the third layer preferably contains a polyvinyl acetal resin (hereinafter sometimes 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. Since the sound insulation is further enhanced, the polyvinyl acetal resin (1) is preferably different from the polyvinyl acetal resin (2) and the polyvinyl acetal resin (3).
  • the thermoplastic resin (1), the thermoplastic resin (2), and the thermoplastic resin (3) may be the same or different.
  • the said polyvinyl acetal resin (1), the said polyvinyl acetal resin (2), and the said polyvinyl acetal resin (3) only 1 type may respectively be used and 2 or more types may be used together.
  • the said thermoplastic resin (1), the said thermoplastic resin (2), and the said thermoplastic resin (3) only 1 type may respectively be used and 2 or more types may be used together.
  • thermoplastic resin examples include polyvinyl acetal resin, polyacrylic resin, ethylene-vinyl acetate copolymer resin, ethylene-acrylic acid copolymer resin, polyurethane resin, and polyvinyl alcohol resin. Thermoplastic resins other than these may be used.
  • the polyvinyl acetal resin is preferably an acetalized product of polyvinyl alcohol.
  • the polyvinyl alcohol can be obtained, for example, by saponifying polyvinyl acetate.
  • the 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 It is 5000 or less, more preferably 4000 or less, and still more preferably 3500 or less.
  • the average degree of polymerization is not less than the above lower limit, the penetration resistance and bending rigidity of the laminated glass are further increased.
  • the average degree of polymerization is not more than the above upper limit, the molded article can be easily molded.
  • the average degree of polymerization of the polyvinyl alcohol is determined by a method based on JIS K6726 “Testing method for polyvinyl alcohol”.
  • the carbon number of the acetal group is preferably 2 to 10, more preferably 2 to 5, and further preferably 2, 3 or 4.
  • the carbon number of the acetal group in the polyvinyl acetal resin is preferably 2 or 4, and in this case, the production of the polyvinyl acetal resin is efficient.
  • an aldehyde having 1 to 10 carbon atoms is suitably used as the aldehyde.
  • the aldehyde having 1 to 10 carbon atoms include formaldehyde, acetaldehyde, propionaldehyde, n-butyraldehyde, isobutyraldehyde, n-valeraldehyde, 2-ethylbutyraldehyde, n-hexylaldehyde, n-octylaldehyde, Examples include n-nonyl aldehyde, n-decyl aldehyde, cumin aldehyde, and benzaldehyde.
  • Acetaldehyde, propionaldehyde, n-butyraldehyde, isobutyraldehyde, n-hexylaldehyde or n-valeraldehyde are preferred. Acetaldehyde, propionaldehyde, n-butyraldehyde, isobutyraldehyde or n-valeraldehyde is more preferred, and acetaldehyde, n-butyraldehyde or n-valeraldehyde is still more preferred. As for the said aldehyde, only 1 type may be used and 2 or more types may be used together.
  • the hydroxyl content (hydroxyl content) of the polyvinyl acetal resin (1) is preferably in the following range.
  • the hydroxyl group content (hydroxyl content) of the polyvinyl acetal resin (1) is preferably 25 mol% or more, more preferably 28 mol% or more, more preferably 30 mol% or more, and even more preferably 31.5 mol%. More preferably, it is at least 32 mol%, particularly preferably at least 33 mol%.
  • the hydroxyl group content (hydroxyl group amount) of the polyvinyl acetal resin (1) is preferably not more than 37 mol%, more preferably not more than 36.5 mol%, still more preferably not more than 36 mol%.
  • the bending rigidity is further increased, and the adhesive strength of the molded body is further increased.
  • the flexibility of a molded object becomes it high that the content rate of the said hydroxyl group is below the said upper limit, and handling of a molded object becomes easy.
  • the hydroxyl group content (hydroxyl content) of the polyvinyl acetal resin (1) is preferably 17 mol% or more, more preferably 20 mol% or more, still more preferably 22 mol% or more, preferably 28 mol% or less, more preferably. Is 27 mol% or less, more preferably 25 mol% or less, and particularly preferably 24 mol% or less.
  • the polyvinyl acetal resin (1) when used as a part of a multilayer molded article, it is preferable that the lower limit and the upper limit of the hydroxyl group content are satisfied.
  • the mechanical strength of a molded object becomes it still higher that the content rate of the said hydroxyl group is more than the said minimum.
  • the reaction efficiency is high and the productivity is excellent, and when it is 28 mol% or less, the sound insulation of the laminated glass is further enhanced. .
  • the flexibility of a molded object becomes it high that the content rate of the said hydroxyl group is below the said upper limit, and handling of a molded object becomes easy.
  • a laminated glass using a molded product having a hydroxyl group content of 28 mol% or less in the polyvinyl acetal resin (1) tends to have a low bending rigidity. Can improve.
  • the content of each hydroxyl group in the polyvinyl acetal resin (2) and the polyvinyl acetal resin (3) is preferably 25 mol% or more, more preferably 28 mol% or more, more preferably 30 mol% or more, and still more preferably. It is 31.5 mol% or more, more preferably 32 mol% or more, and particularly preferably 33 mol% or more.
  • Each content rate of the hydroxyl group of the said polyvinyl acetal resin (2) and the said polyvinyl acetal resin (3) becomes like this. Preferably it is 37 mol% or less, More preferably, it is 36.5 mol% or less, More preferably, it is 36 mol% or less.
  • the hydroxyl group content is at least the above lower limit, the bending rigidity is further increased, and the adhesive strength of the molded body is further increased. Moreover, the flexibility of a molded object becomes it high that the content rate of the said hydroxyl group is below the said upper limit, and handling of a molded object becomes easy.
  • the hydroxyl group content of the polyvinyl acetal resin (1) is preferably lower than the hydroxyl group content of the polyvinyl acetal resin (2). From the viewpoint of further increasing the sound insulation, the hydroxyl group content of the polyvinyl acetal resin (1) is preferably lower than the hydroxyl group content of the polyvinyl acetal resin (3). From the viewpoint of further improving sound insulation, 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.
  • 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, it is 5 mol% or more, 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 indicating the mole fraction obtained by dividing the amount of ethylene groups to which the hydroxyl group is bonded by the total amount of ethylene groups in the main chain, as a percentage.
  • the amount of the ethylene group to which the hydroxyl group is bonded can be measured, for example, according to JIS K6728 “Testing method for polyvinyl butyral”.
  • 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 at least mol%, preferably at most 30 mol%, more preferably at most 25 mol%, still more preferably at most 24 mol%.
  • the degree of acetylation is not less than the above lower limit, the compatibility between the polyvinyl acetal resin and the plasticizer or other thermoplastic resin is increased, the sound insulation and penetration resistance are further improved, and the performance is further improved over a long period of time. Stabilize.
  • the degree of acetylation is not more than the above upper limit, the moisture resistance of the molded body and the laminated glass is increased.
  • 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 improved.
  • Each degree of acetylation of the polyvinyl acetal resin (2) and the polyvinyl acetal resin (3) is preferably 0.01 mol% or more, more preferably 0.5 mol% or more, preferably 10 mol% or less, more preferably. Is 2 mol% or less.
  • the acetylation degree is not less than the above lower limit, the compatibility between the polyvinyl acetal resin and the plasticizer is increased.
  • the degree of acetylation is not more than the above upper limit, the moisture resistance of the molded body and the laminated glass is increased.
  • the degree of acetylation is a value obtained by dividing the amount of ethylene groups to which the acetyl group is bonded by the total amount of ethylene groups in the main chain, as a percentage.
  • the amount of ethylene group to which the acetyl group is bonded can be measured, for example, according to JIS K6728 “Testing method for polyvinyl butyral”.
  • the degree of acetalization 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 It is 85 mol% or less, More preferably, it is 80 mol% or less, More preferably, it is 75 mol% or less.
  • the degree of acetalization is not less than the above lower limit, the compatibility between the polyvinyl acetal resin and the plasticizer increases.
  • the degree of acetalization is less than or equal to the above upper limit, the reaction time required for producing a polyvinyl acetal resin is shortened.
  • the degree of acetalization (degree of butyralization in the case of polyvinyl butyral resin) of the polyvinyl acetal resin (2) and the polyvinyl acetal resin (3) is preferably 55 mol% or more, more preferably 60 mol% or more, preferably Is 75 mol% or less, more preferably 71 mol% or less.
  • degree of acetalization is not less than the above lower limit, the compatibility between the polyvinyl acetal resin and the plasticizer increases.
  • the degree of acetalization is less than or equal to the above upper limit, the reaction time required for producing a polyvinyl acetal resin is shortened.
  • the degree of acetalization is obtained as follows. First, a value obtained by subtracting the amount of ethylene groups bonded with hydroxyl groups and the amount of ethylene groups bonded with acetyl groups from the total amount of ethylene groups in the main chain is obtained. The obtained value is divided by the total amount of ethylene groups in the main chain to obtain the mole fraction. A value indicating the mole fraction as a percentage is the degree of acetalization.
  • the hydroxyl group content (hydroxyl content), acetalization degree (butyralization degree), and acetylation degree are preferably calculated from results measured by a method in accordance with JIS K6728 “Testing methods for polyvinyl butyral”. However, measurement by ASTM D1396-92 may be used.
  • the polyvinyl acetal resin is a polyvinyl butyral resin
  • the hydroxyl group content (hydroxyl amount), the acetalization degree (butyralization degree), and the acetylation degree are determined in accordance with JIS K6728 “Testing methods for polyvinyl butyral”. It can be calculated from the results measured by
  • the molded body preferably contains a plasticizer.
  • the first layer (including a single-layer molded body) preferably contains a plasticizer (hereinafter sometimes referred to as a plasticizer (1)).
  • the second layer preferably contains a plasticizer (hereinafter sometimes referred to as a plasticizer (2)).
  • the third layer preferably contains a plasticizer (hereinafter may be referred to as a plasticizer (3)).
  • a plasticizer 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. As for the said plasticizer (1), the said plasticizer (2), and the said plasticizer (3), only 1 type may respectively be used and 2 or more types may be
  • plasticizer examples include organic ester plasticizers such as monobasic organic acid esters and polybasic organic acid esters, and organic phosphate plasticizers such as organic phosphoric acid plasticizers and organic phosphorous 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 a reaction between glycol and a monobasic organic acid.
  • Examples of the glycol include triethylene glycol, tetraethylene glycol, and tripropylene glycol.
  • Examples of the monobasic organic acid include butyric acid, isobutyric acid, caproic acid, 2-ethylbutyric acid, heptylic acid, n-octylic acid, 2-ethylhexylic acid, n-nonylic acid, and decylic acid.
  • polybasic organic acid ester examples include ester compounds of a polybasic organic acid and an alcohol having a linear or branched structure having 4 to 8 carbon atoms.
  • polybasic organic acid examples include adipic acid, sebacic acid, and azelaic acid.
  • organic ester plasticizer examples include triethylene glycol di-2-ethylpropanoate, triethylene glycol di-2-ethylbutyrate, triethylene glycol di-2-ethylhexanoate, triethylene glycol dicaprylate, Triethylene glycol di-n-octanoate, triethylene glycol di-n-heptanoate, tetraethylene glycol di-n-heptanoate, dibutyl sebacate, dioctyl azelate, dibutyl carbitol adipate, ethylene glycol di-2-ethylbutyrate, 1,3-propylene glycol di-2-ethyl butyrate, 1,4-butylene glycol di-2-ethyl butyrate, diethylene glycol di-2-ethyl butyrate, diethylene glycol di-2-ethyl Hexanoate, dipropylene glycol di-2-ethylbutyrate, triethylene glycol di-2-eth
  • organic phosphate plasticizer examples 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).
  • 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
  • p represents an integer of 3 to 10
  • R1 and R2 in the above formula (1) are each 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 preferably includes triethylene glycol di-2-ethylhexanoate or triethylene glycol di-2-ethylbutyrate, and further includes triethylene glycol di-2-ethylhexanoate. preferable.
  • the molded article does not contain a plasticizer, or the total of 100 parts by weight of the polyvinyl acetal resin and the polymer.
  • the plasticizer is preferably contained in an amount of 10 parts by weight or less (preferably 5 parts by weight or less).
  • the molded body preferably contains a plasticizer, and the plasticizer is added in an amount of 0.01 parts by weight or more with respect to a total of 100 parts by weight of the polyvinyl acetal resin and the polymer. (Preferably 0.1 parts by weight or more).
  • the plastic with respect to 100 parts by weight of the thermoplastic resin (2) (when the thermoplastic resin (2) is a polyvinyl acetal resin (2), 100 parts by weight of the polyvinyl acetal resin (2)).
  • content of an agent (2) be content (2).
  • the plastic relative to 100 parts by weight of the thermoplastic resin (3) (when the thermoplastic resin (3) is a polyvinyl acetal resin (3), 100 parts by weight of the polyvinyl acetal resin (3)).
  • content of an agent (3) be content (3).
  • the content (2) and the content (3) are each preferably 10 parts by weight or more, more preferably 15 parts by weight or more, preferably 40 parts by weight or less, more preferably 35 parts by weight or less, and still more preferably 32 parts.
  • the content (2) and the content (3) are equal to or more than the lower limit, the flexibility of the molded body is increased and the molded body is easily handled.
  • the content (2) and the content (3) are equal to or lower than the upper limit, the bending rigidity is further increased.
  • the plastic relative to 100 parts by weight of the thermoplastic resin (1) (or 100 parts by weight of the polyvinyl acetal resin (1) when the thermoplastic resin (1) is a polyvinyl acetal resin (1)).
  • content of an agent (1) be 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 85 parts by weight or less, more preferably 80 parts by weight or less.
  • the content (1) is not less than the above lower limit, the flexibility of the molded body is increased and the molded body is easily handled.
  • 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.
  • the content (1) is preferably larger than the content (2) in order to enhance the sound insulation of the laminated glass, and the content (1) is It is preferable that there is more than the said content (3).
  • the laminated glass using the molded body having the content (1) of 55 parts by weight or more tends to have low bending rigidity, but the structure of the present invention can remarkably improve the bending rigidity.
  • the absolute value of the difference between the content (2) and the content (1), and the difference between the content (3) and the content (1) is preferably 10 parts by weight or more, more preferably 15 parts by weight or more, and 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 each preferably 80 parts by weight or less. More preferably, it is 75 weight part or less, More preferably, it is 70 weight part or less.
  • the molded body preferably contains a heat shielding material (heat shielding compound).
  • the first layer preferably contains a heat shielding material.
  • the second layer preferably includes a heat shielding material.
  • the third layer preferably contains a heat shielding material. As for the said heat-shielding substance, only 1 type may be used and 2 or more types may be used together.
  • the heat-insulating substance preferably contains at least one component X of phthalocyanine compounds, naphthalocyanine compounds and anthracocyanine compounds, or contains heat-shielding particles. In this case, both the component X and the heat shielding particles may be included.
  • the molded body preferably contains at least one component X of a phthalocyanine compound, a naphthalocyanine compound, and an anthracocyanine compound.
  • the first layer preferably contains the component X.
  • the second layer preferably contains the component X.
  • the third layer preferably contains the component X.
  • the component X is a heat shielding material. As for the said component X, only 1 type may be used and 2 or more types may be used together.
  • the component X is not particularly limited.
  • component X conventionally known phthalocyanine compounds, naphthalocyanine compounds and anthracocyanine compounds can be used.
  • the component X is preferably at least one selected from the group consisting of phthalocyanine, a derivative of phthalocyanine, naphthalocyanine, and a derivative of naphthalocyanine. More preferably, it is at least one of phthalocyanine and phthalocyanine derivatives.
  • the component X preferably contains a vanadium atom or a copper atom.
  • the component X preferably contains a vanadium atom, and preferably contains a copper atom.
  • the component X is more preferably at least one of a phthalocyanine containing a vanadium atom or a copper atom and a phthalocyanine derivative containing a vanadium atom or a copper atom.
  • the component X preferably 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. % By weight or more, more preferably 0.01% by weight or more, particularly preferably 0.02% by weight or more. In 100% by weight of the layer containing the component X (first layer, second layer, or third layer), the content of the component X is preferably 0.2% by weight or less, more preferably 0.1%. % By weight or less, more preferably 0.05% by weight or less, particularly preferably 0.04% by weight or less.
  • 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.
  • the visible light transmittance can be 70% or more.
  • Thermal barrier particles The molded body preferably includes heat shielding particles.
  • the first layer (including a single-layer molded body) preferably includes the heat shielding particles.
  • the second layer preferably includes the heat shielding particles.
  • the third layer preferably contains the heat shielding particles.
  • the heat shielding particles are heat shielding materials. By using heat shielding particles, infrared rays (heat rays) can be effectively blocked. As for the said heat-shielding particle, only 1 type may be used and 2 or more types may be used together.
  • the heat shielding particles are more preferably metal oxide particles.
  • the heat shielding particles are preferably particles (metal oxide particles) formed of a metal oxide.
  • Infrared rays having a wavelength longer than 780 nm longer than visible light have a smaller amount of energy than ultraviolet rays.
  • infrared rays have a large thermal effect, and when infrared rays are absorbed by a substance, they are released as heat. For this reason, infrared rays are generally called heat rays.
  • heat shielding particles By using the heat shielding particles, infrared rays (heat rays) can be effectively blocked.
  • the heat shielding particles mean particles that can absorb infrared rays.
  • heat shielding particles include aluminum-doped tin oxide particles, indium-doped tin oxide particles, antimony-doped tin oxide particles (ATO particles), gallium-doped zinc oxide particles (GZO particles), and indium-doped zinc oxide particles (IZO particles).
  • Aluminum doped zinc oxide particles (AZO particles), niobium doped titanium oxide particles, sodium doped tungsten oxide particles, cesium doped tungsten oxide particles, thallium doped tungsten oxide particles, rubidium doped tungsten oxide particles, tin doped indium oxide particles (ITO particles) And metal oxide particles such as tin-doped zinc oxide particles and silicon-doped zinc oxide particles, and lanthanum hexaboride (LaB 6 ) particles. Heat shielding particles other than these may be used.
  • Metal oxide particles are preferred because of their high heat ray shielding function, ATO particles, GZO particles, IZO particles, ITO particles or tungsten oxide particles are more preferred, and ITO particles or tungsten oxide particles are particularly preferred.
  • 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.
  • the tungsten oxide particles are preferably metal-doped tungsten oxide particles.
  • the “tungsten oxide particles” include metal-doped tungsten oxide particles. Specific examples of the metal-doped tungsten oxide particles include sodium-doped tungsten oxide particles, cesium-doped tungsten oxide particles, thallium-doped tungsten oxide particles, and rubidium-doped tungsten oxide particles.
  • cesium-doped tungsten oxide particles are particularly preferable.
  • the cesium-doped tungsten oxide particles are preferably tungsten oxide particles represented by the formula: Cs 0.33 WO 3 .
  • the average particle diameter of the heat shielding particles is preferably 0.01 ⁇ m or more, more preferably 0.02 ⁇ m or more, preferably 0.1 ⁇ m or less, more preferably 0.05 ⁇ m or less.
  • the average particle size is not less than the above lower limit, the heat ray shielding property is sufficiently increased.
  • the average particle size is not more than the above upper limit, the dispersibility of the heat shielding particles is increased.
  • the above “average particle diameter” indicates the volume average particle diameter.
  • the average particle diameter 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%. .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%. % 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.
  • the molded body preferably contains at least one metal salt (hereinafter sometimes referred to as metal salt M) among alkali metal salts, alkaline earth metal salts, and magnesium salts.
  • the first layer preferably includes the metal salt M.
  • the second layer preferably contains the metal salt M.
  • the third layer preferably contains the metal salt M.
  • Use of the metal salt M makes it easy to control the adhesion between the molded body and the laminated glass member or the adhesion between the layers in the molded body.
  • the said metal salt M only 1 type may be used and 2 or more types may be used together.
  • the metal salt M preferably contains 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 body preferably contains at least one metal 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 it is more preferably a carboxylic acid magnesium salt having 2 to 16 carbon atoms or a carboxylic acid potassium salt having 2 to 16 carbon atoms.
  • Examples of the C 2-16 carboxylic acid magnesium salt and the C 2-16 carboxylic acid potassium salt include magnesium acetate, potassium acetate, magnesium propionate, potassium propionate, magnesium 2-ethylbutyrate, 2-ethylbutanoic acid. Examples include potassium, magnesium 2-ethylhexanoate, and potassium 2-ethylhexanoate.
  • the total content of Mg and K in the layer containing the metal salt M is preferably 5 ppm or more, more preferably 10 ppm or more, and even more preferably 20 ppm or more. , Preferably 300 ppm or less, more preferably 250 ppm or less, still more preferably 200 ppm or less.
  • the adhesion between the molded body and the laminated glass member or the adhesion between the layers in the molded body can be controlled even better.
  • the molded body 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.
  • the ultraviolet shielding agent includes an ultraviolet absorber.
  • the ultraviolet shielding agent is preferably an ultraviolet absorber.
  • the ultraviolet shielding agent examples include an ultraviolet shielding agent containing a metal atom, an ultraviolet shielding agent containing a metal oxide, an ultraviolet shielding agent having a benzotriazole structure (benzotriazole compound), and an ultraviolet shielding agent having a benzophenone structure (benzophenone compound). ), UV screening agent having triazine structure (triazine compound), UV screening agent having malonate ester structure (malonic acid ester compound), UV screening agent having oxalic acid anilide structure (oxalic acid anilide compound) and benzoate structure Examples thereof include an ultraviolet shielding agent (benzoate compound).
  • Examples of the ultraviolet shielding agent containing a metal atom include platinum particles, particles having platinum particles coated with silica, palladium particles, and particles having palladium particles coated with silica.
  • the ultraviolet shielding agent is preferably not a heat shielding particle.
  • the ultraviolet shielding agent is preferably an ultraviolet shielding agent having a benzotriazole structure, an ultraviolet shielding agent having a benzophenone structure, an ultraviolet shielding agent having a triazine structure, or an ultraviolet shielding agent having a benzoate structure.
  • the ultraviolet shielding agent is more preferably an ultraviolet shielding agent having a benzotriazole structure or an ultraviolet shielding agent having a benzophenone structure, and more preferably an ultraviolet shielding agent having a benzotriazole structure.
  • Examples of the ultraviolet shielding agent containing the metal oxide include zinc oxide, titanium oxide, and cerium oxide. Furthermore, the surface may be coat
  • Examples of the ultraviolet screening agent having the benzotriazole structure include 2- (2′-hydroxy-5′-methylphenyl) benzotriazole (“TinvinP” manufactured by BASF), 2- (2′-hydroxy-3 ′, 5′-di-t-butylphenyl) benzotriazole (“Tinvin 320” manufactured by BASF), 2- (2′-hydroxy-3′-t-butyl-5-methylphenyl) -5-chlorobenzotriazole (BASF) And “Tinuvin 326” manufactured by BASF, etc.) and the like.
  • the ultraviolet shielding agent is preferably an ultraviolet shielding agent having a benzotriazole structure containing a halogen atom, and may be an ultraviolet shielding agent having a benzotriazole structure containing a chlorine atom. More preferred.
  • Examples of the ultraviolet shielding agent having the benzophenone structure include octabenzone (“Chimasorb 81” manufactured by BASF).
  • UV shielding agent having the triazine structure examples include “LA-F70” manufactured by ADEKA and 2- (4,6-diphenyl-1,3,5-triazin-2-yl) -5-[(hexyl). Oxy] -phenol (“Tinuvin 1577FF” manufactured by BASF) and the like.
  • UV screening agent having a malonic ester structure examples include dimethyl 2- (p-methoxybenzylidene) malonate, tetraethyl-2,2- (1,4-phenylenedimethylidene) bismalonate, and 2- (p-methoxybenzylidene).
  • 2- (p-methoxybenzylidene) malonate examples include dimethyl 2- (p-methoxybenzylidene) malonate, tetraethyl-2,2- (1,4-phenylenedimethylidene) bismalonate, and 2- (p-methoxybenzylidene).
  • Examples of commercially available ultraviolet screening agents having a malonic ester structure include Hostavin B-CAP, Hostavin PR-25, and Hostavin PR-31 (all manufactured by Clariant).
  • Examples of the ultraviolet shielding agent having the oxalic anilide structure include N- (2-ethylphenyl) -N ′-(2-ethoxy-5-tert-butylphenyl) oxalic acid diamide, N- (2-ethylphenyl)- Oxalic acid diamides having an aryl group substituted on the nitrogen atom such as N ′-(2-ethoxy-phenyl) oxalic acid diamide, 2-ethyl-2′-ethoxy-oxyanilide (“SlandorVSU” manufactured by Clariant)kind.
  • ultraviolet shielding agent having the benzoate structure examples include 2,4-di-tert-butylphenyl-3,5-di-tert-butyl-4-hydroxybenzoate (“Tinuvin 120” manufactured by BASF). .
  • the content of the ultraviolet screening agent is preferably 0.1% by weight or more, more preferably 0%. .2% by weight or more, more preferably 0.3% by weight or more, and particularly preferably 0.5% by weight or more.
  • the content of the ultraviolet shielding agent is preferably 2.5% by weight or less, more preferably 2%. % By weight or less, more preferably 1% by weight or less, particularly preferably 0.8% by weight or less.
  • the content of the ultraviolet shielding agent is not less than the above lower limit and not more than the above upper limit, a decrease in visible light transmittance after a lapse of time can be further suppressed.
  • the content of the ultraviolet shielding agent is 0.2% by weight or more, thereby reducing the visible light transmittance after the passage of the molded body and the laminated glass. Remarkably suppressed.
  • the molded body preferably contains an antioxidant.
  • the first layer preferably contains an antioxidant.
  • the second layer preferably contains an antioxidant.
  • the third layer preferably contains an antioxidant. As for the said antioxidant, only 1 type may be used and 2 or more types may be used together.
  • antioxidants examples include phenol-based antioxidants, sulfur-based antioxidants, and phosphorus-based antioxidants.
  • the phenolic antioxidant is an antioxidant having a phenol skeleton.
  • the sulfur-based antioxidant is an antioxidant containing a sulfur atom.
  • the phosphorus antioxidant is an antioxidant containing a phosphorus atom.
  • the antioxidant is preferably a phenolic antioxidant or a phosphorus antioxidant.
  • phenolic antioxidant examples include 2,6-di-t-butyl-p-cresol (BHT), butylhydroxyanisole (BHA), 2,6-di-t-butyl-4-ethylphenol, stearyl- ⁇ - (3,5-di-t-butyl-4-hydroxyphenyl) propionate, 2,2′-methylenebis- (4-methyl-6-butylphenol), 2,2′-methylenebis- (4-ethyl-6) -T-butylphenol), 4,4'-butylidene-bis- (3-methyl-6-t-butylphenol), 1,1,3-tris- (2-methyl-hydroxy-5-t-butylphenyl) butane Tetrakis [methylene-3- (3 ′, 5′-butyl-4-hydroxyphenyl) propionate] methane, 1,3,3-tris- (2-methyl-4-hydro) Loxy-5-t-butylphenol) butane, 1,3,5-trimethyl-2,4,6
  • Examples of the phosphorus antioxidant include tridecyl phosphite, tris (tridecyl) phosphite, triphenyl phosphite, trinonylphenyl phosphite, bis (tridecyl) pentaerythritol diphosphite, bis (decyl) pentaerythritol diphos.
  • antioxidants examples include “IRGANOX 245” manufactured by BASF, “IRGAFOS 168” manufactured by BASF, “IRGAFOS 38” manufactured by BASF, “Smilizer BHT” manufactured by Sumitomo Chemical Co., Ltd., and Sakai Chemical Industry Examples thereof include “H-BHT” and “IRGANOX 1010” manufactured by BASF.
  • a layer in 100% by weight of the molded body or containing an antioxidant.
  • the content of the antioxidant is preferably 0.1% by weight or more.
  • the content of the antioxidant is preferably 2% by weight or less in 100% by weight of the molded body or 100% by weight of the layer containing the antioxidant.
  • the molded body, the first layer, the second layer, and the third layer are respectively a coupling agent containing silicon, aluminum, or titanium, a dispersant, a surfactant, a flame retardant, Additives such as antistatic agents, fillers, pigments, dyes, adhesive strength modifiers, moisture-proofing agents, fluorescent brighteners and infrared absorbers may be included. As for these additives, only 1 type may be used and 2 or more types may be used together.
  • the molded body, the first layer, the second layer, and the third layer may contain a filler.
  • 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 is preferably 1% by weight or more, more preferably 5% by weight or more, and still more preferably. It is 10 weight part or more, Preferably it is 60 weight% or less, More preferably, it is 50 weight% or less.
  • the thickness of the molded body is not particularly limited. From the viewpoint of practical use and from the viewpoint of sufficiently increasing 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, more Preferably it is 1.5 mm or less. When the thickness of the molded body is not less than the above lower limit, the penetration resistance and bending rigidity of the laminated glass are further increased. When the thickness of the molded body is not more than the above upper limit, the transparency of the molded body is further improved.
  • the thickness of the intermediate film is T.
  • the thickness of the first layer is preferably 0.035T or more, more preferably 0.0625T or more, further preferably 0.1T or more, preferably 0.4T or less, more preferably 0.375T or less, and still more preferably. It is 0.25 T or less, particularly preferably 0.15 T or less.
  • the thickness of the first layer is 0.4 T or less, the bending rigidity is further improved.
  • Each thickness of the second layer and the third layer is preferably 0.3 T or more, more preferably 0.3125 T or more, still more preferably 0.375 T or more, preferably 0.97 T or less, more preferably 0. 9375T or less, more preferably 0.9T or less.
  • Each thickness of the second layer and the third layer may be 0.46875T or less, or 0.45T or less. Further, when the thicknesses of the second layer and the third layer are not less than the lower limit and not more than the upper limit, the rigidity and sound insulation of the laminated glass are further enhanced.
  • the total thickness of the second layer and the third layer is preferably 0.625 T or more, more preferably 0.75 T or more, still more preferably 0.85 T or more, preferably 0.97 T or less, more preferably 0.9375T or less, more preferably 0.9T or less. Further, when the total thickness of the second layer and the third layer is not less than the above lower limit and not more than the above upper limit, the rigidity and sound insulation of the laminated glass are further enhanced.
  • the intermediate film may be an intermediate film having a uniform thickness or an intermediate film having a changed thickness.
  • the cross-sectional shape of the intermediate film may be rectangular or wedge-shaped.
  • the method for producing the molded body according to the present invention is not particularly limited.
  • Examples of the method for producing a molded body according to the present invention include a method of extruding a resin composition using an extruder in the case of a single-layer molded body.
  • a method for producing a molded body according to the present invention in the case of a multilayer molded body, for example, a method of laminating each obtained layer after forming each layer using each resin composition for forming each layer
  • a method of laminating each layer by coextruding each resin composition for forming each layer using an extruder may be used. Since it is suitable for continuous production, an extrusion method is preferred.
  • the same polyvinyl acetal resin is contained in the second layer and the third layer because the production efficiency of the molded body is excellent. Since the production efficiency of the intermediate film is excellent, it is more preferable that the same polyvinyl acetal resin and the same plasticizer are contained in the second layer and the third layer. Since the production efficiency of the intermediate film is excellent, it is more preferable that the second layer and the third layer are formed of the same resin composition.
  • the molded body preferably has an uneven shape on at least one of the surfaces on both sides. It is more preferable that the molded body has an uneven shape on both surfaces. It does not specifically limit as a method of forming said uneven
  • the embossing roll method is preferable because it can form a large number of concavo-convex embossments that are quantitatively constant.
  • FIG. 3 is a cross-sectional view schematically showing an example of a laminated glass using the laminated glass interlayer film shown in FIG.
  • the intermediate film 11 is disposed between the first laminated glass member 21 and the second laminated glass member 22 and is sandwiched.
  • the first laminated glass member 21 is laminated on the first surface 11 a of the intermediate film 11.
  • a second laminated glass member 22 is laminated on the second surface 11 b opposite to the first surface 11 a of the intermediate film 11.
  • a first laminated glass member 21 is laminated on the outer surface 2 a of the second layer 2.
  • a second laminated glass member 22 is laminated on the outer surface 3 a of the third layer 3.
  • FIG. 4 is a cross-sectional view schematically showing an example of laminated glass using the interlayer film for laminated glass shown in FIG.
  • a laminated glass 31A shown in FIG. 4 includes a first laminated glass member 21, a second laminated glass member 22, and an intermediate film 11A.
  • 11 A of intermediate films are arrange
  • the first laminated glass member 21 is laminated on the first surface 11a of the intermediate film 11A.
  • a second laminated glass member 22 is laminated on the second surface 11b opposite to the first surface 11a of the intermediate film 11A.
  • the laminated glass which concerns on this invention is equipped with the 1st laminated glass member, the 2nd laminated glass member, and a molded object (intermediate film), and this molded object (intermediate film) is this book. It is the molded object which concerns on invention.
  • the said molded object is arrange
  • the first laminated glass member is preferably a first glass plate.
  • the second laminated glass member is preferably a second glass plate.
  • the laminated glass member examples 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 laminate including a glass plate, and preferably at least one glass plate is used.
  • Each of the first laminated glass member and the second laminated glass member is a glass plate or a PET film, and the laminated glass is one of the first laminated glass member and the second laminated glass member. It is preferable to provide a glass plate as at least one.
  • the glass plate examples include inorganic glass and organic glass.
  • the inorganic glass examples include float plate glass, heat ray absorbing plate glass, heat ray reflecting plate glass, polished plate glass, mold plate glass, and wire-containing plate glass.
  • the organic glass is a synthetic resin glass that replaces the inorganic glass.
  • examples of the organic glass include polycarbonate plates and poly (meth) acrylic resin plates.
  • Examples of the poly (meth) acrylic resin plate include a polymethyl (meth) acrylate plate.
  • the thickness of the laminated glass member is preferably 1 mm or more, preferably 5 mm or less, more preferably 3 mm or less.
  • 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, more preferably 3 mm or less.
  • the thickness of the PET film is preferably 0.03 mm or more, and preferably 0.5 mm or less.
  • the use of the molded body according to the present invention can maintain the bending rigidity of the laminated glass high even if the laminated glass is thin.
  • the thickness of the glass plate is preferably 2 mm or less, more preferably 1.8 mm or less, even more preferably 1.6 mm or less, still more preferably 1.5 mm or less, still more preferably 1.4 mm or less, and even more preferably 1. 0.3 mm or less, still more preferably 1.0 mm or less, and particularly preferably 0.7 mm or less.
  • the laminated glass can be reduced in weight
  • the environmental load can be reduced by reducing the material of the laminated glass
  • the environmental load can be reduced by improving the fuel efficiency of the automobile by reducing the weight of the laminated glass. .
  • the total thickness of the first glass plate and 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, particularly preferably 2.8 mm or less. It is.
  • the laminated glass can be reduced in weight
  • the environmental load can be reduced by reducing the material of the laminated glass
  • the environmental load can be reduced by improving the fuel efficiency of the automobile by reducing the weight of the laminated glass. .
  • 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 laminate. Next, for example, the obtained laminated body is passed through a pressing roll or put in a rubber bag and sucked under reduced pressure, whereby the first laminated glass member, the second laminated glass member, and the molded body. The remaining air is deaerated. Thereafter, pre-bonding is performed at about 70 to 110 ° C. to obtain a pre-bonded laminate. Next, the pre-pressed laminate is put in an autoclave or pressed and pressed at about 120 to 150 ° C. and a pressure of 1 to 1.5 MPa. In this way, a laminated glass can be obtained. You may laminate
  • the molded body and the laminated glass can be used for automobiles, railway vehicles, aircraft, ships, buildings, and the like.
  • the said molded object and the said laminated glass can be used besides these uses.
  • the molded body and the laminated glass are preferably a molded body and laminated glass for vehicles or buildings, and more preferably an interlayer film and laminated glass for vehicles.
  • the said molded object and the said laminated glass can be used for the windshield, side glass, rear glass, roof glass, etc. of a motor vehicle.
  • the said molded object and the said laminated glass are used suitably for a motor vehicle.
  • the said molded object is used in order to obtain the laminated glass of a motor vehicle.
  • Polyvinyl acetal resin Polyvinyl acetal resins shown in Tables 1 to 3 below were appropriately used.
  • the degree of acetalization, the degree of acetylation, and the hydroxyl group content were measured by a method in accordance with JIS K6728 “Testing methods for polyvinyl butyral”. In addition, when measured by ASTM D1396-92, the same numerical value as the method based on JIS K6728 “Testing method for polyvinyl butyral” was shown. Further, when the type of acetal is acetoacetal, benzyl acetal or cumin acetal, the degree of acetal is similarly measured for the degree of acetylation and the content of hydroxyl groups, and the molar fraction is determined from the obtained measurement results. Calculated, and then calculated by subtracting the degree of acetylation and the hydroxyl group content from 100 mol%.
  • the acrylic polymers shown in Tables 1 to 3 below are acrylic polymers obtained by polymerizing polymerizable components containing the following compounds in the contents shown in Tables 1 to 3 below.
  • Ethyl acrylate butyl acrylate benzyl acrylate 2-hydroxyethyl acrylate acrylic acid glycidyl methacrylate tripropylene glycol diacrylate (“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.) ⁇ -Caprolactone-modified tris- (2-acryloxyethyl) isocyanurate (“A-9300-1CL” manufactured by Shin-Nakamura Chemical Co., Ltd.) Tris phosphate [2- (acryloyloxy) ethyl] Ethoxylated pentaerythritol
  • Example 1 A polyvinyl acetal resin (average polymerization degree 560, acetalization degree 74.0 mol%, hydroxyl group content 25.0 mol%, acetylation degree 0.9 mol%) was prepared. 100 parts by weight of a 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, and 0.6 parts by weight of tripropylene glycol diacrylate) were prepared.
  • a 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, and 0.6 parts by weight of tripropylene glycol diacrylate
  • 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.
  • the polyvinyl acetal resin was dissolved while stirring.
  • nitrogen gas was blown for 30 minutes to replace the inside of the reaction vessel with nitrogen, and then the reaction vessel was heated to 80 ° C. while stirring.
  • 3GO as a plasticizer
  • diluted solvent mixed solvent of methanol and toluene, methanol and toluene, was diluted 1: 2
  • this solution was applied onto a PET film that had been subjected to a mold release treatment using a coater so that the thickness after drying was 50 ⁇ m, and dried at 80 ° C. for 1 hour to obtain an intermediate film.
  • the obtained intermediate film having a thickness of 50 ⁇ m was superposed and subjected to thermocompression bonding at 150 ° C. and 20 MPa to obtain an intermediate film having a thickness of 400 ⁇ m.
  • 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.
  • the diameter (maximum diameter) of the island part 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.
  • A The average diameter of the islands is 10 nm or more and 1 ⁇ m or less.
  • B Does not correspond to the standard of A.
  • Break strength is 40 MPa or more ⁇ : Break strength is 30 MPa or more and less than 40 MPa ⁇ : Break strength is 20 MPa or more and less than 30 MPa ⁇ : Break strength is less than 20 MPa

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  • Chemical & Material Sciences (AREA)
  • Health & Medical Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Medicinal Chemistry (AREA)
  • Polymers & Plastics (AREA)
  • Organic Chemistry (AREA)
  • Laminated Bodies (AREA)
  • Joining Of Glass To Other Materials (AREA)
  • Adhesive Tapes (AREA)
  • Polymerisation Methods In General (AREA)
  • Graft Or Block Polymers (AREA)
  • Adhesives Or Adhesive Processes (AREA)
  • Compositions Of Macromolecular Compounds (AREA)

Abstract

L'invention concerne un corps moulé capable d'améliorer l'allongement à la rupture à des températures basses et des vitesses élevées, et capable d'améliorer la résistance à la rupture à des températures basses et à des vitesses élevées. Un corps moulé selon la présente invention est pourvu d'une structure de séparation de phase qui comprend une résine d'acétal de polyvinyle, et un polymère d'un composant polymérisable comprenant un composé (méth)acrylate ayant deux groupes (méth)acryloyle ou plus. La teneur du polymère est d'au moins 85 mais pas plus de 180 parties en poids pour 100 parties en poids de la résine d'acétal de polyvinyle.
PCT/JP2018/013336 2017-03-31 2018-03-29 Corps moulé et verre feuilleté Ceased WO2018181755A1 (fr)

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JP2021155725A (ja) * 2020-03-27 2021-10-07 積水化学工業株式会社 ポリビニルアセタール樹脂
JPWO2020111153A1 (ja) * 2018-11-30 2021-11-04 昭和電工マテリアルズ株式会社 車両用合わせガラス
KR20220019695A (ko) 2019-06-11 2022-02-17 세키스이가가쿠 고교가부시키가이샤 수지 조성물, 수지 필름, 및 유리 적층체

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WO2015046583A1 (fr) * 2013-09-30 2015-04-02 積水化学工業株式会社 Film intermédiaire pour verre feuilleté, et verre feuilleté
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