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WO2015040663A1 - Feuille contenant de l'acétal de polyvinyle - Google Patents

Feuille contenant de l'acétal de polyvinyle Download PDF

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Publication number
WO2015040663A1
WO2015040663A1 PCT/JP2013/074971 JP2013074971W WO2015040663A1 WO 2015040663 A1 WO2015040663 A1 WO 2015040663A1 JP 2013074971 W JP2013074971 W JP 2013074971W WO 2015040663 A1 WO2015040663 A1 WO 2015040663A1
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WO
WIPO (PCT)
Prior art keywords
sheet
silicon
plasticizer
polyvinyl acetal
layer
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/JP2013/074971
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English (en)
Japanese (ja)
Inventor
芳聡 浅沼
三原　一郎
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Kuraray Co Ltd
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Kuraray Co Ltd
Priority date (The priority date 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 date listed.)
Filing date
Publication date
Application filed by Kuraray Co Ltd filed Critical Kuraray Co Ltd
Priority to PCT/JP2013/074971 priority Critical patent/WO2015040663A1/fr
Priority to JP2013544918A priority patent/JP5503088B1/ja
Publication of WO2015040663A1 publication Critical patent/WO2015040663A1/fr
Anticipated expiration legal-status Critical
Ceased legal-status Critical Current

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    • 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
    • C08K5/54—Silicon-containing compounds
    • 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
    • B32B17/10005—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 laminated safety glass or glazing
    • B32B17/1055—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 laminated safety glass or glazing characterized by the resin layer, i.e. interlayer
    • B32B17/10761—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 laminated safety glass or glazing characterized by the resin layer, i.e. interlayer containing vinyl acetal
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08J—WORKING-UP; GENERAL PROCESSES OF COMPOUNDING; AFTER-TREATMENT NOT COVERED BY SUBCLASSES C08B, C08C, C08F, C08G or C08H
    • C08J5/00—Manufacture of articles or shaped materials containing macromolecular substances
    • C08J5/18—Manufacture of films or sheets
    • 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
    • C08K5/0008—Organic ingredients according to more than one of the "one dot" groups of C08K5/01 - C08K5/59
    • C08K5/0016—Plasticisers
    • 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
    • C08K5/09—Carboxylic acids; Metal salts thereof; Anhydrides thereof
    • C08K5/098—Metal salts of carboxylic acids
    • 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
    • C08K5/101—Esters; Ether-esters of monocarboxylic acids
    • C08K5/103—Esters; Ether-esters of monocarboxylic acids with polyalcohols
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08J—WORKING-UP; GENERAL PROCESSES OF COMPOUNDING; AFTER-TREATMENT NOT COVERED BY SUBCLASSES C08B, C08C, C08F, C08G or C08H
    • C08J2329/00—Characterised by the use 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; Hydrolysed polymers of esters of unsaturated alcohols with saturated carboxylic acids; Derivatives of such polymer
    • C08J2329/14—Homopolymers or copolymers of acetals or ketals obtained by polymerisation of unsaturated acetals or ketals or by after-treatment of polymers of unsaturated alcohols

Definitions

  • the present invention relates to a sheet containing polyvinyl acetal and its use.
  • a sheet made of polyvinyl acetal and a plasticizer is widely used as an interlayer film for laminated glass because of its excellent adhesion and transparency to glass and mechanical strength.
  • a high-boiling plasticizer is preferable from the viewpoint of suppressing the volatilization of the plasticizer when used over a long period of time or at a high temperature.
  • a high-boiling plasticizer is preferable from the viewpoint of suppressing the volatilization of the plasticizer when used over a long period of time or at a high temperature.
  • triethylene glycol di-2-ethylhexanoate (3GO) is widely used in recent years because it has a high boiling point, is compatible with polyvinyl acetal, and is excellent in the plasticizing effect of polyvinyl acetal.
  • 3GO is a low polarity compound, and a sheet containing polyvinyl acetal and 3GO tends to be easily charged.
  • a sheet containing polyvinyl acetal and 3GO may be adjusted to a relatively high water content, for example, about 0.5 to 0.9%, and stored in a state that is difficult to be charged. .
  • the adhesion between the interlayer film for laminated glass and the glass must be appropriately adjusted according to the purpose.
  • a method of adjusting the adhesion between the interlayer film for laminated glass and the glass a method of adding an alkali metal salt of carboxylic acid, an alkaline earth metal salt of carboxylic acid or the like to the interlayer film for laminated glass is known (for example, see Patent Documents 1 to 3.)
  • the carboxylate is a salt of a carboxylic acid having a small carbon number
  • Water absorption may cause the edge of the laminated glass to whiten.
  • Patent Documents 1 to 3 disclose an interlayer film for laminated glass in which a carboxylic acid and a metal salt of a carboxylic acid are used in combination. When such an interlayer film is used, the problem of the change in adhesiveness with time is described. On the other hand, hydrolysis of polyvinyl acetal occurred using carboxylic acid, which is an essential component, as a catalyst, and odor problems sometimes occurred due to the generated aldehyde. Such an odor problem is particularly noticeable when the interlayer film is stored at a relatively high water content.
  • silicon-containing compounds such as silicone oil (see, for example, Patent Documents 4 to 7) and silane coupling agents (see, for example, Reference Documents 8 to 10)
  • silicone oil see, for example, Patent Documents 4 to 7
  • silane coupling agents see, for example, Reference Documents 8 to 10.
  • the silicon-containing compound such as silicone oil or a silane coupling agent
  • the silicon-containing compound is applied to the surface of the interlayer film or kneaded into the interlayer film.
  • these interlayer films are stored for a long time under high humidity, for example, in the case of an interlayer film for laminated glass coated with a silicon-containing compound, the silicon-containing compound moves into the interlayer film over time. Therefore, the interlayer film for laminated glass stored for a long time may not exhibit the same adhesion to glass as the interlayer film before storage.
  • the silicon-containing compound when the silicon-containing compound is kneaded and used in the intermediate film, when such an intermediate film is stored for a long period of time, the silicon-containing compound is gelled in the intermediate film, and the appearance of the laminated glass obtained using this, In particular, the appearance when intense light such as an automobile headlight is irradiated may be impaired.
  • JP 05-186250 A Japanese Patent Application Laid-Open No. 07-041340 Japanese Patent Laid-Open No. 08-119687 JP 50-121311 A Japanese Patent Laid-Open No. 10-139499 JP 2000-007386 A JP 2000-203899 A Japanese Patent Application Laid-Open No. 07-068054 JP 07-237942 A Japanese Patent Laid-Open No. 08-026786
  • This invention provides the sheet
  • the object includes a polyvinyl acetal, a plasticizer having a molecular weight of 380 or more, and a silicon-containing compound, and the plasticizer having a molecular weight of 380 or more is 30 to 70 parts by weight with respect to 100 parts by weight of the polyvinyl acetal.
  • the sheet is 0.2 to 2 mm and 0.10 to 30 ppm of silicon is detected when the sheet is analyzed by ICP emission spectrometry, and TOF-SIMS measurement is performed in a cross section parallel to the thickness direction of the sheet
  • the total number of silicon secondary ions detected from a region having a thickness of 0 to 60 ⁇ m and a width of W ⁇ m from at least one surface of the sheet is N (0 to 60), and 10 to 10 from the surface in the thickness direction.
  • the total number of silicon secondary ions detected from the region of 60 ⁇ m and width W ⁇ m is N (10 to 60), and 60 to 110 ⁇ m in the thickness direction from the surface and width W ⁇ m.
  • the sheet preferably contains an alkali metal salt and / or an alkaline earth metal salt.
  • the alkali metal salt and / or alkaline earth metal salt is preferably an alkali metal salt of carboxylic acid or an alkaline earth metal salt of carboxylic acid.
  • the carboxylic acid is preferably a carboxylic acid having 1 to 8 carbon atoms.
  • the content of the alkali metal salt and / or alkaline earth metal salt is preferably 0.001 to 0.1 parts by mass with respect to 100 parts by mass of the polyvinyl acetal.
  • the silicon-containing compound is preferably a compound containing a silicon-oxygen bond.
  • the silicon-containing compound is preferably a silane coupling agent.
  • the silicon-containing compound is preferably silicone oil.
  • the plasticizer having a molecular weight of 380 or more is preferably triethylene glycol di-2-ethylhexanoate.
  • the total storage time at a temperature exceeding 30 ° C. is preferably less than 3000 hours.
  • the difference is preferably 0 to 500.
  • Silicon contained in sheet A obtained by laminating sheet A containing polyvinyl acetal, a plasticizer having a molecular weight of 380 or more and a silicon-containing compound, and sheet B containing polyvinyl acetal, a plasticizer having a molecular weight of 380 or more and a silicon-containing compound
  • concentration of the contained compound is higher than the concentration of the silicon-containing compound contained in the sheet B, and the difference between the degree of acetalization of the polyvinyl acetal contained in the sheet A and the degree of acetalization of the polyvinyl acetal contained in the sheet B is 0 to 3 mol%. It is preferable that
  • Silicon contained in sheet A obtained by laminating sheet A containing polyvinyl acetal, a plasticizer having a molecular weight of 380 or more and a silicon-containing compound, and sheet B containing polyvinyl acetal, a plasticizer having a molecular weight of 380 or more and a silicon-containing compound
  • concentration of the contained compound is higher than the concentration of the silicon-containing compound contained in the sheet B, and the difference between the average residual hydroxyl group amount of the polyvinyl acetal contained in the sheet A and the average residual hydroxyl group amount of the polyvinyl acetal contained in the sheet B is 0-3. It is preferable that it is mol%.
  • Silicon contained in sheet A obtained by laminating sheet A containing polyvinyl acetal, a plasticizer having a molecular weight of 380 or more and a silicon-containing compound, and sheet B containing polyvinyl acetal, a plasticizer having a molecular weight of 380 or more and a silicon-containing compound the concentration of the containing compound is higher than the concentration of the silicon-containing compound contained in the sheet B, and highest plasticizer content of the plasticizer contained in the sheet a and the plasticizer a 1, often a second content plasticizer agent and plasticizer a 2, the content of the plasticizer a 1 with respect to 100 parts by mass of the polyvinyl acetal contained in the sheet a and (a 1) part by weight, the content of the plasticizer a 2 for the polyvinyl acetal 100 parts by (a 2) as a mass parts, further, the highest plasticizer content of the plasticizer contained in the sheet B and a plasticizer B 1, the content of two More plasticizer to the eye as a plasticizer B 2, the content of
  • the object includes a polyvinyl acetal, a plasticizer having a molecular weight of 380 or more, and a silicon-containing compound, and the plasticizer having a molecular weight of 380 or more is 30 to 70 parts by weight with respect to 100 parts by weight of the polyvinyl acetal.
  • the sheet is 0.2 to 2 mm and 0.10 to 30 ppm of silicon is detected when the sheet is analyzed by ICP emission spectrometry, and TOF-SIMS measurement is performed in a cross section parallel to the thickness direction of the sheet
  • the total number of silicon secondary ions detected from a region having a thickness of 0 to X ⁇ m and a width of W ⁇ m from at least one surface of the sheet is N (0 to X), and X /
  • the total number of silicon secondary ions detected from the region of 6 to X ⁇ m and width W ⁇ m is N (X / 6 to X), and X to 11X / 6 ⁇ m and width W ⁇ m in the thickness direction from the surface.
  • 5/6 ⁇ N (0 to X) / N (X to 11X / 6) is 1.2 or more when the total number of silicon secondary ions detected from the region is N (X to 11X / 6) 5/6 ⁇ N (0 to X) / N (X / 6 to X) is 0.8 to 2, and X is 20 to 90 ⁇ m, and can be suitably achieved by providing a sheet .
  • the above object is suitably achieved by providing a laminated glass including the sheet.
  • the silicon 2 when TOF-SIMS measurement is performed in a cross section parallel to the thickness direction of the sheet, the silicon 2 detected from a region having a thickness of 0 to 60 ⁇ m and a width of W ⁇ m from at least one surface of the sheet.
  • the total number of secondary ions is N (0 to 60), the total number of silicon secondary ions detected from the surface in the thickness direction of 10 to 60 ⁇ m and the width W ⁇ m is N (10 to 60),
  • N the total number of silicon secondary ions detected from the region having a thickness of 60 to 110 ⁇ m and a width of W ⁇ m from the surface
  • 5/6 ⁇ N (0 to 60) / N ( 60 to 110) is 1.2 or more, which is 0 to 60 ⁇ m in the thickness direction from the surface of the sheet as compared to the inside of the sheet represented by the region of 60 to 110 ⁇ m in the thickness direction from the surface of the sheet.
  • Sheet surface represented by area In the vicinity, the silicon-containing compound at a high concentration represents a be distributed.
  • the adhesiveness to the glass is appropriately achieved by the action of the silicon-containing compound present at a high concentration in the vicinity of the sheet surface.
  • the problem of appearance due to the gelation of the silicon-containing compound can be suppressed while adjusting to the above.
  • 5/6 ⁇ N (0 to 60) / N (10 to 60) is 0.8 to 2. This is in the vicinity of the sheet surface in the thickness direction from the surface.
  • the concentration of the silicon-containing compound existing in the region of 0 to 60 ⁇ m and the portion excluding the region of 0 to 10 ⁇ m out of the region of 0 to 60 ⁇ m in the thickness direction from the surface, that is, 10 to 60 ⁇ m in the thickness direction from the surface indicates that the concentration of the silicon-containing compound existing in the region does not change significantly.
  • the adhesive force changes even when the sheet of the present invention is stored for a long period of time. Is unlikely to occur.
  • the polyvinyl acetal used in the present invention is not particularly limited, and the degree of polymerization, the degree of acetalization, the average residual hydroxyl group amount, and the vinyl ester residue amount are not particularly limited.
  • the viscosity average polymerization degree is preferably 200 to 3000, more preferably 500 to 2400, and more preferably 1000 to 2000. More preferably.
  • the processability of the sheet of the present invention may be reduced, and when the viscosity average degree of polymerization is less than 200, the mechanical strength of the obtained sheet may be reduced, or silicon content may be reduced. Compound migration tends to occur.
  • the degree of acetalization of polyvinyl acetal is not particularly limited, but is preferably 40 to 85 mol%, more preferably 60 to 80 mol%, and further preferably 67 to 75 mol%. If the degree of acetalization is less than 40 mol%, the flexibility of the resulting sheet will be insufficient, and the compatibility with plasticizers and silicon-containing compounds having a molecular weight of 380 or more contained in the sheet will be reduced, resulting in transparency. May decrease.
  • the average residual hydroxyl group content of polyvinyl acetal is preferably 10 to 50 mol%, more preferably 19 to 39 mol%, and further preferably 24 to 32 mol%.
  • the compatibility with a plasticizer having a molecular weight of 380 or more may be lowered, and when it is less than 10 mol%, the mechanical strength of the resulting sheet may be lowered.
  • the amount of vinyl ester residue of polyvinyl acetal is preferably 0.01 to 20 mol%, more preferably 0.1 to 10 mol%, and further preferably 0.2 to 3 mol%. Those having a vinyl ester residue content of less than 0.01 mol% are difficult to produce industrially at low cost, and those having a vinyl ester residue content of more than 20 mol% are those having a vinyl ester residue during long-term storage.
  • the group may be hydrolyzed to generate, for example, carboxylic acid such as acetic acid, and the carboxylic acid may be used as a catalyst to hydrolyze the polyvinyl acetal to generate an aldehyde that causes odor.
  • the polyvinyl acetal used in the present invention is produced using, for example, a polyvinyl alcohol that can be obtained by a conventionally known method or a conventionally known modified polyvinyl alcohol as a raw material.
  • the polyvinyl acetal used in the present invention is produced by a conventionally known method. For example, first, an aqueous solution of polyvinyl alcohol having a concentration of 3 to 40% by mass is maintained in a temperature range of 80 to 100 ° C., and then the aqueous solution is gradually cooled over 10 to 60 minutes. When the temperature drops to ⁇ 10 to 30 ° C., an aldehyde and an acid catalyst are added, and an acetalization reaction is performed for 30 to 300 minutes while keeping the temperature constant. At that time, polyvinyl alcohol having a certain degree of acetalization is deposited. Thereafter, the reaction solution is heated to a temperature of 30 to 80 ° C. over 30 to 300 minutes, and the temperature is maintained for 10 to 500 minutes. Next, a basic compound is added to the reaction solution, the acid catalyst is neutralized, washed with water, and dried to obtain polyvinyl acetal.
  • the acid catalyst used in the acetalization reaction is not particularly limited, and any of organic acids and inorganic acids can be used. Examples thereof include acetic acid, paratoluenesulfonic acid, nitric acid, sulfuric acid, hydrochloric acid and the like. Of these, hydrochloric acid, sulfuric acid, and nitric acid are preferably used.
  • the aldehyde used in the acetalization reaction is not particularly limited, but acetalization with a conventionally known aldehyde having 1 to 8 carbon atoms is preferable, and an aldehyde having 4 to 6 carbon atoms is preferable, and n-butyraldehyde is particularly preferable. Is preferably used.
  • the polyvinyl acetal obtained by using together 2 or more types of aldehydes can also be used, and 2 or more types of polyvinyl acetals obtained using different aldehydes can also be mixed and used.
  • the plasticizer having a molecular weight of 380 or more used in the present invention is not particularly limited.
  • triethylene glycol di-2-ethylhexanoate (3GO, molecular weight 402)
  • tetraethylene glycol di-2-ethylhexanoate (4GO, molecular weight 446).
  • Aliphatic ester compounds such as dinonyl adipate (molecular weight 398), dioctyl sebacate (molecular weight 426), aromatic ester compounds such as dioctyl phthalate (molecular weight 396), adipic acid and 3-methyl-1
  • a conventionally known polyester compound having a molecular weight of 380 or more such as a polyester compound obtained by copolymerization with 5-pentanediol, can be used.
  • those having a molecular weight of 380 to 2000 are preferred, those having a molecular weight of 390 to 1000 are more preferred, and those having a molecular weight of 400 to 600 are more preferred.
  • the silicon-containing compound contained as an essential component in the present invention quickly shifts to the inside of the sheet (in the sheet thickness direction, the same applies hereinafter), thereby achieving the object of the present invention. I can't.
  • the molecular weight of the plasticizer exceeds 2000, the compatibility with the polyvinyl acetal is poor, the transparency of the resulting sheet may be impaired, and the plasticizing effect on the polyvinyl acetal is not sufficiently exhibited. There is.
  • the chemical structure of the plasticizer of the present invention is not particularly limited, but from the viewpoint of appropriately adjusting the adhesion between the sheet of the present invention and glass, at least one functional group selected from a hydrocarbon group, an ether bond and an ester bond.
  • a plasticizer containing only groups is preferred.
  • the plasticizer used in the present invention is triethylene glycol di-2-ethylhexanoate because it is difficult for the silicon-containing compound to move into the sheet and is excellent in compatibility with polyvinyl acetal and plasticizing effect on polyvinyl acetal. It is best to be an eate.
  • the plasticizer content is preferably 30 to 70 parts by weight, more preferably 31 to 60 parts by weight, and more preferably 32 to 50 parts by weight with respect to 100 parts by weight of polyvinyl acetal. More preferably it is. If the plasticizer content is less than 30 parts by mass, the flexibility of the sheet may not be sufficient, and if the plasticizer content is more than 70 parts by mass, the strength and transparency of the sheet may be reduced. There is a tendency that the silicon-containing compound contained in is easily transferred into the sheet.
  • the sheet A and the sheet B are laminated to obtain the sheet of the present invention, the same is applied to the entire sheet with respect to 100 parts by mass of the polyvinyl acetal included in the entire sheet composed of the sheet A and the sheet B.
  • the plasticizer content is preferably 30 to 70 parts by mass.
  • the silicon-containing compound used in the present invention is not particularly limited as long as it does not contradict the gist of the present invention, but a compound containing a silicon-oxygen bond is preferable from the viewpoint of adjusting the adhesion to glass, and in particular, a silane coupling agent. Silicone oil or the like is preferably used.
  • the silane coupling agent is not particularly limited, but methyltrimethoxysilane, hexyltrimethoxysilane, phenyltrimethoxysilane, 3-aminopropyltrimethoxysilane, 3-aminopropyltriethoxysilane, 3-glycidyloxypropyltrimethoxysilane
  • conventionally known silane coupling agents such as 3-glycidyloxypropyltriethoxysilane, vinyltrimethoxysilane, and 3-methacryloxypropyltrimethoxysilane.
  • those having an epoxy group or an amino group are particularly preferable from the viewpoint of adjusting the adhesive force with glass.
  • silicone oil examples include conventionally known silicone oils such as dimethyl silicone, methylphenyl silicone, amino group-modified silicone, alkyl group-modified silicone, polyether group-modified silicone, and carboxyl group-modified silicone. Amino group-modified silicone, polyether group-modified silicone, and carboxyl group-modified silicone are preferred from the viewpoint of adjusting the adhesion to glass.
  • the silicon content in the sheet of the present invention is 0.10 to 30 ppm, preferably 0.20 to 25 ppm, preferably 0.30 to 20 ppm, when analyzed by ICP emission spectrometry. More preferred.
  • the silicon content is less than 0.10 ppm as the silicon detection amount when the sheet is analyzed by ICP emission spectrometry, the effect of adjusting the adhesive force is insufficient, and when the silicon detection amount exceeds 30 ppm,
  • the silicon-containing compound may gel and the appearance of the resulting laminated glass may be impaired.
  • the content of silicon in the sheet of the present invention was determined by cutting a sheet sample in a plane parallel to the cross section in the thickness direction, adding sulfuric acid and nitric acid, thermally decomposing, and then using a solution with a constant volume of hydrochloric acid. And it can carry out by measuring with an ICP emission spectrometer (Optima4300DV by Perkin Elmer).
  • the TOF-SIMS measurement of the sheet can be performed by the method described in the examples using, for example, the apparatus described in the examples.
  • the sheet of the present invention when TOF-SIMS measurement is performed on a cross section parallel to the thickness direction of the sheet, silicon 2 detected from a region having a thickness of 0 to X ⁇ m and a width of W ⁇ m from at least one surface of the sheet.
  • the total number of secondary ions is N (0 to X)
  • the total number of silicon secondary ions detected from the region of X / 6 to X ⁇ m and width W ⁇ m in the thickness direction from the surface is N (X / 6 to X).
  • N (X to 11X / 6)
  • 5/6 ⁇ N (0 to X) / N (X to 11X / 6) is 1.2 or more
  • 5/6 ⁇ N (0 to X) / N (X / 6 to X) is 0.8 to 2.
  • X can be appropriately designed according to the thickness of the sheet, and is 20 to 90 ⁇ m, preferably 20 to 80 ⁇ m.
  • a region formed of a W ⁇ m rectangle is a region to be measured by TOF-SIMS measurement.
  • the sheet of the present invention is detected from a region to be measured (hereinafter referred to as a measurement target region) 2a (refer to FIG. 1A) having a thickness of 0 to 60 ⁇ m and a width W ⁇ m from at least one surface of the sheet 1.
  • the total number of silicon secondary ions to be detected is N (0 to 60), and is detected from the measurement target region 2b (see FIG.
  • N 10 to 60
  • silicon secondary ions detected from the measurement target region 2c (see FIG. 1C) having a thickness of 60 to 110 ⁇ m and a width of W ⁇ m from the surface.
  • 5/6 ⁇ N (0-60) / N (60-110) is 1.2 or more, where N is the total number of N (60-110).
  • 5/6 ⁇ N (0 to 60) / N (60 to 110) is preferably 1.3 to 20, more preferably 1.4 to 10, and more preferably 1.5 to 8. Further preferred.
  • the area of the measurement target region 2c of N (60 to 110) is 5/6 times the area of the measurement target region 2a of N (0 to 60), and is 5/6 ⁇ N (0 to 60) / N
  • the value “5/6” in (60 to 110) is a coefficient for correcting the difference in area between the two regions.
  • 5/6 ⁇ N (0 to 60) / N (10 to 60) is 0.8 to 2, but preferably 0.83 to 1.7, and 0.85 to 1.5. More preferably, it is most preferably 0.9 to 1.3.
  • 5/6 ⁇ N (0 to 60) / N (10 to 60) is less than 0.8 or more than 2, when the obtained sheet is stored for a long period of time, the adhesion to glass is It may change and is not preferable.
  • the area of the measurement target region 2b of N (10 to 60) is 5/6 times the area of the measurement target region 2a of N (0 to 60), and is 5/6 ⁇ N (0 to 60) / N
  • the value “5/6” in (10 to 60) is a coefficient for correcting the difference in area between the two regions.
  • W is an arbitrary positive number and is preferably 10 to 1000 ⁇ m.
  • N 10 to 60
  • N 60 to 110
  • TOF-SIMS measurement is performed with a uniform width W ⁇ m.
  • the sheet of the present invention may contain an alkali metal salt and / or an alkaline earth metal salt from the viewpoint of optimizing the adhesiveness with glass, as long as it does not contradict the gist of the present invention.
  • the alkali metal salt and alkaline earth metal salt are not particularly limited, and a cation selected from alkali metal ions such as sodium ion and potassium ion, or alkaline earth metal ions such as magnesium ion and calcium ion, acetate ion and propane Acid ion, butanoic acid ion, 2-ethylhexylic acid ion, 2-ethyl-2-hexenoic acid ion, nonanoic acid ion, decanoic acid ion, stearic acid ion, oleic acid ion, carboxylate ion such as adipic acid ion, chlorine ion
  • an alkali metal salt of a carboxylic acid or an alkaline earth metal salt of a carboxylic acid is particularly preferable from the viewpoint of appropriately adjusting the adhesiveness between the sheet of the present invention and glass.
  • an alkali metal salt of a carboxylic acid having 1 to 8 carbon atoms, preferably 1 to 4 carbon atoms, more preferably 2 to 3 carbon atoms, or 1 to 8 carbon atoms, preferably 1 to 4 carbon atoms, more preferably Alkaline earth metal salts of carboxylic acids having 2 to 3 carbon atoms are preferred from the viewpoint that the adhesion between the sheet and the glass hardly changes even when the sheet of the present invention is used for a long time.
  • an alkaline earth metal salt having 2 to 3 carbon atoms is particularly preferable in that it has an excellent whitening suppression effect upon water absorption.
  • the content of the alkali metal salt and / or alkaline earth metal salt in the sheet of the present invention is not particularly limited, but is 100 parts by weight of polyvinyl acetal.
  • the amount is preferably 0.001 to 0.1 parts by mass, more preferably 0.001 to 0.07 parts by mass, and still more preferably 0.001 to 0.05 parts by mass.
  • the content of the alkali metal salt and / or alkaline earth metal salt is less than 0.001 part by mass, the effect of adjusting the adhesiveness between the sheet of the present invention and the glass may not be sufficiently exhibited.
  • the content of the salt and / or alkaline earth metal salt exceeds 0.1 parts by mass, the sheet of the present invention is likely to be whitened by water absorption, which is not preferable.
  • the sheet of the present invention may contain an antioxidant, an ultraviolet absorber, and other additives as long as it is not contrary to the gist of the present invention.
  • an antioxidant for example, a conventionally known sheet can be used.
  • the amount added can also be appropriately selected according to the purpose.
  • the method for producing the sheet of the present invention is not particularly limited, for example, a method of laminating layers A and B having different concentrations of the silicon-containing compound may be mentioned. More preferably, the method of laminating
  • the concentration of the silicon-containing compound contained in the layer A is preferably 1.2 times or more, more preferably 1.3 to 20 times the concentration of the silicon-containing compound contained in the layer B. It is more preferable to set it to ⁇ 10 times, and it is optimal to set it to 1.5 to 8 times.
  • the thickness of the layer A is preferably 20 to 90 ⁇ m, more preferably 40 to 70 ⁇ m, further preferably 55 to 70 ⁇ m, and most preferably 57 to 65 ⁇ m.
  • the thickness of the layer B is preferably 50 to 1900 ⁇ m, more preferably 300 to 1200 ⁇ m, and even more preferably 500 to 1000 ⁇ m.
  • the contained compound is distributed at a high concentration, and the silicon-containing compound has a region of 0 to 60 ⁇ m in the thickness direction from the sheet surface on the layer A side and a region of 10 to 60 ⁇ m in the thickness direction from the sheet surface on the layer A side. It is possible to obtain a sheet whose density does not change greatly, that is, a sheet defined in the present invention.
  • a sheet defined in the present invention When layer A / layer B / layer A are stacked in this order, the requirements specified in the present invention can be satisfied in any region specified from any surface.
  • the content of the plasticizer having a molecular weight of 380 or more in the layer A is preferably 30 to 70 parts by mass, and more preferably 31 to 60 parts by mass with respect to 100 parts by mass of the polyvinyl acetal. Further, the content of the silicon-containing compound in the layer A is preferably 0.002 to 0.3 parts by mass, and preferably 0.003 to 0.25 parts by mass with respect to 100 parts by mass of the polyvinyl acetal. More preferred.
  • the adhesive strength with the glass cannot be adjusted appropriately, and the content of the silicon-containing compound in the layer A Is more than 0.3 parts by mass, when the obtained sheet is stored for a long period of time, the silicon-containing compound is transferred to the inside of the sheet, the adhesiveness with the glass is likely to change, the silicon-containing compound Gelation tends to impair the appearance.
  • the content of the plasticizer having a molecular weight of 380 or more in the layer B is preferably 30 to 70 parts by mass, and more preferably 31 to 60 parts by mass with respect to 100 parts by mass of the polyvinyl acetal.
  • the content of the silicon-containing compound in the layer B is preferably 0.0001 to 0.02 parts by mass, and preferably 0.0005 to 0.01 parts by mass with respect to 100 parts by mass of the polyvinyl acetal. More preferred.
  • the silicon-containing compound in the layer B is less than 0.0001 parts by mass with respect to 100 parts by mass of the polyvinyl acetal, the silicon-containing compound moves into the sheet when the obtained sheet is stored for a long period of time. The adhesiveness to glass tends to change, and if it exceeds 0.02 parts by mass, the silicon-containing compound gels and the appearance tends to be impaired.
  • the concentration of the silicon-containing compound contained in the layer D is preferably 1.2 times or more the concentration of the silicon-containing compound contained in the layer C, more preferably 1.3 to 20 times, More preferably, it is 1.4 to 10 times, and most preferably 1.5 to 8 times.
  • the thickness of the layer C is preferably 50 to 1900 ⁇ m, preferably 300 to 1200 ⁇ m, and more preferably 500 to 1000 ⁇ m.
  • the thickness of the layer D is preferably 20 to 90 ⁇ m, more preferably 40 to 70 ⁇ m, still more preferably 55 to 70 ⁇ m, and most preferably 57 to 65 ⁇ m.
  • concentration and thickness of the silicon-containing compound in layers C and D are not limited to these.
  • the layer D may be formed on one surface of the layer C, or the layer D may be formed on both surfaces of the layer C. By forming the layer D on one surface of the layer C, in the region of 0 to 60 ⁇ m in the thickness direction from the surface on the layer D side, compared to the region of 60 to 110 ⁇ m in the thickness direction from the surface on the layer D side.
  • the silicon-containing compound is distributed at a high concentration, and the concentration of the silicon-containing compound in the region of 0 to 60 ⁇ m in the thickness direction from the surface on the layer D side and in the region of 10 to 60 ⁇ m in the thickness direction from the surface on the layer D side Can be obtained, that is, a sheet defined by the present invention.
  • the layer D is formed on both surfaces of the layer C, the requirements defined in the present invention can be satisfied in the region specified from any surface.
  • the content of the plasticizer having a molecular weight of 380 or more in the layer C is preferably 30 to 70 parts by mass, and more preferably 31 to 60 parts by mass with respect to 100 parts by mass of the polyvinyl acetal. Further, the content of the silicon-containing compound in the layer C is preferably 0.0001 to 0.02 parts by mass, and preferably 0.0005 to 0.01 parts by mass with respect to 100 parts by mass of the polyvinyl acetal. More preferred. When the content of the silicon-containing compound in the layer C is less than 0.0001 parts by mass with respect to 100 parts by mass of the polyvinyl acetal, the silicon-containing compound moves into the sheet when the obtained sheet is stored for a long period of time. The adhesiveness to glass tends to change, and if it exceeds 0.02 parts by mass, the silicon-containing compound gels and the appearance tends to be impaired.
  • Examples of the coating solution used for forming the layer D include 30 to 70 parts by mass of a plasticizer having a molecular weight of 380 or more, 0.002 to 0.3 parts by mass of a silicon-containing compound, and 1000 parts by mass based on 100 parts by mass of polyvinyl acetal. It is preferable that it contains ⁇ 5000 parts by mass of solvent.
  • the content of the silicon-containing compound in the layer D is more preferably 0.005 to 0.25 parts by mass with respect to 100 parts by mass of the polyvinyl acetal.
  • the silicon-containing compound in the layer D When the content of the silicon-containing compound in the layer D is more than 0.3 parts by mass with respect to 100 parts by mass of the polyvinyl acetal, the silicon-containing compound moves into the sheet when the resulting sheet is stored for a long period of time. As a result, the adhesiveness to glass tends to change, and the silicon-containing compound tends to gel and the appearance tends to be impaired.
  • the solvent used in the coating solution for forming the layer D is not particularly limited as long as it can dissolve polyvinyl acetal, and examples thereof include tetrahydrofuran, chloroform, ethanol, propanol, butanol, and the like. Of these, ethanol and propanol are preferred.
  • the coating solution for forming layer D is preferably applied so that the thickness of layer D when dried is 20 to 90 ⁇ m, more preferably 40 to 70 ⁇ m, and 55 It is more preferable to apply so as to have a thickness of 70 ⁇ m.
  • the sheet of the present invention is a laminate of layer A and layer B or a laminate of layer C and layer D
  • the polyvinyl acetal, plasticizer, and silicon-containing compound are defined in the present invention. Needless to say, it meets the requirements.
  • the sheet of the present invention is preferably produced by the former method. Further, even in the former method, when the layers A and B are laminated, if the temperature is heated to 120 ° C. or higher, the silicon-containing compound may move in the sheet thickness direction. It is preferable that the temperature be less than 120 ° C.
  • the difference between the viscosity average polymerization degree of the polyvinyl acetal contained in the portion of 0 to 60 ⁇ m from the surface of the sheet and the viscosity average polymerization degree of the polyvinyl acetal contained in the portion of 60 to 110 ⁇ m is 0 to 500. It is preferably 0, more preferably 0 to 300, still more preferably 0 to 200, and most preferably 0 to 100. It is preferable that the difference in the viscosity average polymerization degree satisfies such a range because when the sheet of the present invention is stored for a long period of time, the silicon-containing compound does not easily move into the sheet.
  • the difference between the degree of acetalization of the polyvinyl acetal contained in the layer A and the degree of acetalization of the polyvinyl acetal contained in the layer B is preferably 0 to 3 mol%, and preferably 0 to 2 mol%. More preferably, it is 0 to 1 mol%. Further, the difference between the average residual hydroxyl group content of polyvinyl acetal contained in layer A and the average residual hydroxyl group content of polyvinyl acetal contained in layer B is preferably 0-3 mol%, and 0-2 mol%. More preferred is 0 to 1 mol%.
  • the polyvinyl acetal contained in the sheet of the present invention satisfies such a range, when the sheet of the present invention is stored for a long period of time, it is difficult for the silicon-containing compound contained as an essential component to move into the sheet. Is preferred.
  • the highest content of high plasticizer and plasticizer A 1 also to more plasticizer Second plasticizer A 2
  • the content of plasticizer A 1 with respect to 100 parts by mass of polyvinyl acetal in layer A is (a 1 ) parts by mass
  • the content of plasticizer A 2 with respect to 100 parts by mass of polyvinyl acetal in layer A is (a 2 ) parts by mass.
  • plasticizers for polyvinyl acetal 100 parts by weight of the layer B the content of B 1 and (b 1) part by weight, when the content of the plasticizer B 2 with respect to the polyvinyl acetal 100 parts by weight of the layer B and (b 2) parts by weight, (a 2) / a 1) and (b 2) / (preferably b 1) are both 0 and 0.1, more preferably 0 to 0.07 and more preferably 0 to 0.05.
  • the thickness of the sheet of the present invention is 200 to 2000 ⁇ m (0.2 to 2 mm), preferably 500 to 1500 ⁇ m, and more preferably 700 to 1300 ⁇ m.
  • the adhesiveness to glass is the same as when using a sheet before long-term storage, although it is suitable because it exhibits an appearance, in order to better exhibit the effects of the present invention, a temperature exceeding 30 ° C., preferably a temperature exceeding 25 ° C., more preferably a temperature exceeding 20 ° C. after the production of the sheet. Those stored at a low temperature such that the total storage time at is less than 3000 hours are more preferred.
  • the storage time at a temperature exceeding 30 ° C. is preferably less than 2000 hours, and more preferably less than 1000 hours. When the storage time at a temperature exceeding 30 ° C. is 3000 hours or more, the silicon-containing compound contained as an essential component in the sheet of the present invention may migrate, and the intended characteristics of the present invention may not be exhibited.
  • the glass laminated with the sheet is not particularly limited.
  • inorganic glass such as float plate glass, polished plate glass, mold plate glass, mesh plate glass, heat ray absorbing plate glass
  • organic glasses such as methyl methacrylate and polycarbonate can be used, and these may be colorless, colored, transparent or non-transparent, but inorganic glass is more preferable. These may be used alone or in combination of two or more.
  • the thickness of the glass is not particularly limited, but is preferably 20 mm or less, more preferably 10 mm or less, and even more preferably 5 mm or less. Further, a part or all of the organic glass or inorganic glass used in the laminated glass may be replaced with a polyester sheet or the like.
  • the shape of the outermost surface of the sheet is not particularly limited, and it may be smooth or may have a concavo-convex structure.
  • the method for producing laminated glass is not particularly limited, and can be produced by a conventionally known method.
  • a method using a vacuum laminator device, a vacuum Examples include a method using a bag, a method using a vacuum ring, a method using a nip roll, and the like.
  • lamination is performed at a temperature of 100 to 200 ° C., preferably 130 to 160 ° C. under a reduced pressure of 1 ⁇ 10 ⁇ 6 to 3 ⁇ 10 ⁇ 2 MPa.
  • a method using a vacuum bag or a vacuum ring is described in, for example, European Patent No. 1235683, and is laminated at 130 to 145 ° C. under a pressure of about 2 ⁇ 10 ⁇ 2 MPa, for example.
  • an example of the operating condition is as follows: a method of first press-bonding at a temperature not higher than the flow start temperature of polyvinyl acetal plasticized with a plasticizer, and then temporarily pressing at a temperature close to the flow start temperature Is mentioned.
  • a method of heating to 30 to 70 ° C. with an infrared heater and the like, degassing with a roll, further heating to 50 to 120 ° C., and then pressing with a roll to bond or temporarily bond may be mentioned.
  • the operating conditions of the autoclave process that is additionally performed after the temporary pressure bonding are appropriately selected according to the thickness and configuration of the module and the laminated glass.
  • the operating conditions are 130 to 130 at a pressure of 1.0 to 1.5 MPa (gauge pressure).
  • the treatment is carried out at a temperature of ⁇ 145 ° C. for 0.5 to 3 hours.
  • the reaction solution was heated to 66 ° C., held at 66 ° C. for 100 minutes, and then cooled to room temperature.
  • the acid catalyst was neutralized with an aqueous sodium hydroxide solution, further washed with ion-exchanged water, dehydrated and dried to obtain polyvinyl butyral (PVB-1).
  • the resulting PVB-1 had a butyralization degree (average acetalization degree) of 70.1 mol%, a residual vinyl acetate group content of 0.9 mol%, and an average residual hydroxyl group content of 29 mol%. .
  • the degree of butyralization of PVB-1 and the content of the remaining vinyl acetate groups were measured according to JIS K6728. The measurement results are shown in Table 1.
  • PVB-2 Polyvinyl butyral (PVB-2) was obtained in the same manner as in the preparation of PVB-1, except that the amount of butyraldehyde used was changed to 195 g and the holding time at 66 ° C. was changed to 190 minutes.
  • the degree of butyralization (average degree of acetalization) of PVB-2 was 74.5 mol%, the content of residual vinyl acetate groups was 0.9 mol%, and the average amount of residual hydroxyl groups was 24.6 mol%.
  • the degree of butyralization of PVB-2 and the content of residual vinyl acetate groups were measured according to JIS K6728. The measurement results are shown in Table 1.
  • PVB-3 Polyvinyl butyral (PVB-3) was obtained in the same manner as in the preparation of PVB-1, except that the amount of butyraldehyde used was changed to 175 g and the holding time at 66 ° C. was changed to 90 minutes.
  • the degree of butyralization (average degree of acetalization) of PVB-3 was 68.0 mol%, the content of residual vinyl acetate groups was 0.9 mol%, and the average amount of residual hydroxyl groups was 31.1 mol%.
  • the degree of butyralization of PVB-3 and the content of residual vinyl acetate groups were measured according to JIS K6728. The measurement results are shown in Table 1.
  • Example 1 100 parts by weight of PVB-1, 39 parts by weight of triethylene glycol di-2-ethylhexanoate, 0.03 parts by weight of magnesium acetate tetrahydrate, BHT (3,5-t-butyl-4-hydroxytoluene) 0.1 part by mass, 0.03 part by mass of benzotriazole-based ultraviolet absorber (manufactured by BASF, TINUVIN 328) and 0.02 part by mass of 3-glycidyloxypropyltrimethoxysilane were melt-kneaded at 150 ° C. Composition-1A was obtained.
  • Composition-1B was obtained in the same manner as Composition-1A, except that the amount of 3-glycidyloxypropyltrimethoxysilane added was 0.005 parts by mass.
  • a layer-1A having a thickness of 60 ⁇ m is prepared as a sheet A by hot pressing composition-1A at 150 ° C.
  • a layer having a thickness of 680 ⁇ m is formed as sheet B by hot pressing composition-1B at 150 ° C.
  • -1B was laminated in the order of layer-1A / layer-1B / layer-1A, and hot-pressed at 100 ° C. under a pressure of 40 kg / cm 2 for 5 minutes to obtain a sheet-1 having a thickness of 800 ⁇ m.
  • the silicon contained in Sheet-1 was measured by ICP emission analysis and found to be 5.2 ppm.
  • the ICP emission analysis of the silicon amount was conducted by adding sulfuric acid and nitric acid to the PVB-1 sample and thermally decomposing it, and then using a solution with a constant volume of hydrochloric acid and using an ICP emission analyzer (Optima 4300 DV manufactured by Perkin Elmer). This was done by measuring (hereinafter the same). The results are shown in Table 3.
  • the obtained sheet-1 was cut with a microtome in a direction parallel to the thickness direction of the cross section.
  • the cross section in the thickness direction of the obtained sheet-1 is 0 from the surface to the thickness direction.
  • the total number N (0-60) of silicon secondary ions detected from the region of 0 to 60 ⁇ m in the thickness direction and 128 ⁇ m in the width direction, detected from the region of 10 to 60 ⁇ m in the thickness direction and 128 ⁇ m in the width direction The total number of silicon secondary ions N (10 to 60) and the total number N (60 to 110) of silicon secondary ions detected from the region having a thickness of 60 to 110 ⁇ m and a width of 128 ⁇ m are obtained. 5/6 ⁇ N (0 to 60) / N (60 to 110) and 5/6 ⁇ N (0 to 60) / N (10 to 60) were obtained, respectively.
  • the results are shown in Table 3.
  • Sheet-1 was stored at 23 ° C. and 50% RH. After 0 hours from the start of storage (that is, before storage immediately after obtaining a sheet by hot pressing), after 300 hours, after 500 hours, and after 3000 hours, the sheet-1 is adhered to glass by the method described later. And the transparency was evaluated.
  • Sheet-1 was conditioned at 23 ° C. and 28% RH for 24 hours to adjust the moisture content to 0.5%.
  • 2 mm thick float glass is stacked so as to be float glass / sheet-1 / float glass, put into a vacuum bag, treated at 100 ° C. and ⁇ 0.09 MPa (gauge pressure), and temporarily adhered,
  • Laminated glass 1-1 was obtained by processing at 140 ° C. and 1.2 MPa (gauge pressure) in an autoclave.
  • the laminated glass 1-1 was allowed to stand at a temperature of ⁇ 18 ° C. for 24 hours, and then smashed with a hammer having a head weight of 0.45 kg until the particle diameter of the glass became 6 mm or less.
  • the glass piece peeled off from the interlayer film (sheet-1) was shaken off, and the Pummel value was determined according to the criteria shown in Table 2 based on the exposure degree (%) of the interlayer film. It shows that the adhesiveness with respect to the glass plate of a plasticization film is so high that a Pummel value is large.
  • the degree of exposure is the ratio of the area of the portion where the glass piece is peeled and the intermediate film is exposed to the entire area of the intermediate film. The results are shown in Table 4.
  • Sheet-1 was conditioned at 23 ° C. and 28% RH for 24 hours to adjust the moisture content to 0.5%.
  • 2 mm thick float glass is stacked so as to be float glass / sheet-1 / float glass, put into a vacuum bag, treated at 100 ° C. and ⁇ 0.09 MPa (gauge pressure), and temporarily adhered,
  • Laminated glass 1-2 was obtained by an autoclave treatment at 140 ° C. and 1.2 MPa (gauge pressure). The appearance of the obtained laminated glass 1-2 was visually confirmed under an illuminance of 500 lux.
  • the laminated glass 1-2 was irradiated with 2000 candela light from a distance of 30 cm, and the state was visually confirmed. A case where no foreign matter was found in both cases was designated as A, a case where foreign matter was seen only when 2000 candela light was irradiated, and a case where foreign matter was seen in both cases was designated as C.
  • the results are shown in Table 4.
  • Example 2 to 29 Sheets 2 to -29 were prepared in the same manner as in Example 1 except that the composition was changed to the composition shown in Table 3, and evaluated in the same manner as in Example 1. The results are shown in Tables 3 and 4.
  • Comparative Example Sheets 3 to 7 and Comparative Example Sheet-10 were respectively prepared in the same manner as in Example 1 except that the compositions shown in Table 5 were changed, and the same evaluation as in Example 1 was performed. The results are shown in Tables 5 and 6.

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  • Health & Medical Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Medicinal Chemistry (AREA)
  • Polymers & Plastics (AREA)
  • Organic Chemistry (AREA)
  • Engineering & Computer Science (AREA)
  • Manufacturing & Machinery (AREA)
  • Materials Engineering (AREA)
  • Laminated Bodies (AREA)
  • Manufacture Of Macromolecular Shaped Articles (AREA)
  • Joining Of Glass To Other Materials (AREA)
  • Compositions Of Macromolecular Compounds (AREA)

Abstract

L'objet de la présente invention est de fournir une feuille qui est produite en faisant appel à un plastifiant ayant un point de d'ébullition élevé et une faible polarité, et qui a une teneur en eau relativement élevée, et qui, lorsqu'elle est utilisée comme film intermédiaire pour un verre combiné après stockage pendant une longue période, peut avoir une adhérence au verre et un aspect qui sont identiques à ceux obtenus avant le stockage de ladite feuille. La présente invention concerne une feuille comprenant de l'acétal de polyvinyle, un plastifiant ayant une masse moléculaire supérieure ou égale à 380 et un composé contenant du silicium, le plastifiant ayant une masse moléculaire supérieure ou égale à 380 étant présent en une proportion allant de 30 à 70 parties en masse par rapport aux 100 parties en masse d'acétal de polyvinyle et l'épaisseur de la feuille étant comprise entre 0,2 et 2 mm. Lorsque la feuille est analysée par un procédé de spectrométrie d'émission à plasma à couplage inductif (ICP), une teneur allant de 0,10 à 30 ppm de silicium est détectée. Lorsqu'une section transversale de la feuille, qui est définie selon une direction qui est parallèle à la direction de l'épaisseur de la feuille, est soumise à une spectrométrie de masse des ions secondaires à temps de vol (TOF-SIMS), le nombre d'ions secondaires de silicium détectés satisfait à une condition spécifiée.
PCT/JP2013/074971 2013-09-17 2013-09-17 Feuille contenant de l'acétal de polyvinyle Ceased WO2015040663A1 (fr)

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