JP5406594B2 - Method for producing ethylene-unsaturated ester copolymer film for forming laminate - Google Patents

Description

  The present invention relates to a method for producing an ethylene-unsaturated ester copolymer film for forming a laminate, such as an interlayer film for laminated glass and a sealing film for solar cell, and is particularly effective for preventing blocking during film storage. The present invention relates to a method for producing a film having a good tack (a force to adhere to an adherend with a light force in a short time) necessary for positioning in a laminating process.

  Conventionally, a film made of a composition containing an ethylene-unsaturated ester copolymer such as ethylene vinyl acetate copolymer (hereinafter abbreviated as EVA) (hereinafter abbreviated as ethylene-unsaturated ester copolymer film) is combined. It is used for forming a laminate in the form of an intermediate film for glass or a sealing film for solar cell. When an ethylene-unsaturated ester copolymer film is used as an interlayer film for laminated glass, it is sandwiched between glass plates and exhibits functions such as penetration resistance and prevention of scattering of broken glass. In such a case, it is disposed on the front and back surfaces of the solar cell, and exhibits functions such as ensuring insulation and ensuring mechanical durability.

  In the case of producing laminated glass, for example, as shown in FIG. 2, a laminate obtained by disposing the intermediate film 5 between the two glass plates 7A and 7B is pre-pressed under reduced pressure, and each layer is laminated. After deaeration of the air remaining on the substrate, the laminate is bonded and integrated by heat-pressing and bonding.

  Moreover, when manufacturing a solar cell, generally, as shown in FIG. 3, the surface side transparent protective member 11 which consists of a glass plate etc., the surface side sealing film 13A, solar cell cells 14, such as a silicon power generation element, The laminated body in which the back surface side sealing film 13B and the back surface side protection member (back cover) 12 are formed in this order is pre-pressed under reduced pressure, air remaining in each layer is deaerated, and then heated and pressurized to be on the surface side. The sealing film 13A and the back surface side sealing film 13B are cured by cross-linking and integrated.

  Such an ethylene-unsaturated ester copolymer film does not cause a phenomenon in which the films adhere to each other during storage (referred to as blocking), and is a laminate when producing a laminate such as laminated glass or a solar cell. It is required that the workability of the process is good and that the deaeration property in the preliminary pressure bonding process is good. When deaeration is insufficient, the transparency of the resulting laminated glass will decrease, the power generation efficiency of the solar cell will deteriorate, the durability will be insufficient, and bubbles will be generated during long-term use. There is a fear.

  As an ethylene-unsaturated ester copolymer film that meets these requirements, an interlayer film for laminated glass and a sealing film for solar cells, in which a fine concavo-convex pattern (called embossing) is formed on one or both sides of the film, have been developed. (Patent Documents 1 and 2). Also, for example, as a method for producing a film having embossed on both sides, a surface roughness of a pair of embossed rolls (referring to a roll for embossing the film) on one side and the other side. A manufacturing method (Patent Document 3) that defines the relationship between roll temperature and pressing pressure has been developed.

JP 2001-130931 A JP 2002-185027 A Japanese Patent Laid-Open No. 7-178812

  However, the ethylene-unsaturated ester copolymer film provided with these embossings is effective for preventing blocking during storage and improving deaeration of the laminate during production. Not necessarily good. That is, in order to improve the workability of the laminating process, there is a tack (a force that adheres to the adherend in a short time with a light force) that allows the film to be accurately positioned and laminated on a glass plate or the like. Although necessary, tack is reduced by embossing, so that it becomes slippery at the time of lamination, and accurate positioning becomes difficult.

  As a countermeasure for this, it is conceivable to use a film with embossed on only one side and perform positioning in the laminating process on the surface opposite to the surface with embossed (hereinafter abbreviated as non-embossed surface). According to the study, it was found that a non-embossed surface having a good tack could not be obtained even if a film having embossed only on one surface was produced.

  Accordingly, an object of the present invention is a method for producing an ethylene-unsaturated ester copolymer film used for forming a laminate, which is provided with an embossing effective for preventing blocking during film storage, and the like. It is providing the manufacturing method of the film which has the favorable tack required for the positioning in a lamination process.

The object is to insert a film made of a composition containing an ethylene-unsaturated ester copolymer between an embossing roll having a fine concavo-convex shape pattern and a rubber pressing roll disposed opposite to the embossing roll , In the method for manufacturing a film for forming a laminate, which includes a step of transferring embossing only to one surface of the film by pressing the embossing roll against the film, the arithmetic average roughness Ra of the surface of the rubber pressing roll is It is achieved by a manufacturing method characterized by being 0.5 to 1.5 μm.

In general, when embossing is applied only to one side of a resin film, a method is adopted in which the embossing roll is inserted between an embossing roll for transferring the embossing and a pressing roll disposed opposite to the embossing roll, and the embossing roll is pressed against the film. Yes. Usually, the pressing roll is made of rubber having a predetermined elasticity in order to sufficiently transfer the uneven pattern of the embossing roll to the resin film. Until now, various methods for adjusting the surface state of a surface to which embossing is applied (hereinafter referred to as an embossing surface) have been studied, including a method for embossing on both sides as in Patent Document 3. . However, when embossing is imparted only to one side, the resulting surface state of the non-embossed surface has hardly been studied.

  Normally, rubber press rolls are not as smooth as the metal surface due to the nature of the material, and there are fine irregularities, so the fine irregularities may be transferred to the surface of the non-embossed surface. . The inventors set the arithmetic average roughness Ra of the surface of the rubber pressure roll when transferring the emboss to the above range, thereby transferring the emboss sufficiently to the embossed surface and achieving good tack. It has been found that a non-embossed surface can be obtained.

The preferable aspect of the manufacturing method of the film for laminated body formation concerning this invention is as follows.
(1) The fine unevenness | corrugation is formed in the surface opposite to the surface where the embossing of the said film for laminated body formation was transcribe | transferred, and the average space | interval Sm of the said unevenness | corrugation is 600-1600 micrometers.
(2) The arithmetic average roughness Ra of the surface opposite to the surface to which the emboss is transferred of the film for forming a laminate is 1.0 to 2.2 μm.

As above-mentioned, the fine unevenness | corrugation may be formed in the non-embossed surface of the film for laminated body obtained by the manufacturing method of this invention by a rubber | gum press roll as a result. If the average interval Sm of the irregularities and / or the arithmetic average roughness Ra of the surface are within the above ranges, a non-embossed surface having a better tack can be obtained.
(3) The ethylene-unsaturated ester copolymer is an ethylene-vinyl acetate copolymer.
(4) The vinyl acetate content of the ethylene-vinyl acetate copolymer is 20 to 35 parts by mass with respect to 100 parts by mass of the ethylene-vinyl acetate copolymer.
(5) The laminate-forming film is an interlayer film for laminated glass or a sealing film for solar cells. Since the film for forming a laminate obtained by the present invention has a good tack on the non-embossed surface, it is particularly suitable as an interlayer film for laminated glass and a sealing film for solar cells that require accurate positioning during lamination. It is valid.

  According to the method for producing an ethylene-unsaturated ester copolymer film for forming a laminate of the present invention, embossing effective for preventing blocking during storage and improving deaeration during production of the laminate is provided, and a laminating step. Can produce a laminate-forming film having a good tack necessary for positioning in an intermediate film for laminated glass and a sealing film for solar cells, etc., which have excellent adhesion and excellent workability during production, etc. Can be provided.

The typical example of the manufacturing method of the ethylene-unsaturated ester copolymer film for laminated body formation concerning this invention is shown, (A) is a schematic sectional drawing which shows the whole, (B) is a roll and a film. It is the schematic sectional drawing which expanded the contact part (dashed-line part of FIG. 1 (A)). It is a schematic sectional drawing for demonstrating a general laminated glass. It is a schematic sectional drawing for demonstrating a common solar cell.

  Below, the manufacturing method of the ethylene-unsaturated ester copolymer film for laminated body formation of this invention is demonstrated, referring drawings. FIG. 1A is a schematic cross-sectional view showing a typical example of the production method of the present invention, and FIG. 1B is an enlarged schematic cross-sectional view of a contact portion between a roll and a film.

As shown in FIG. 1 (A), first, a film 30 made of a composition containing an ethylene-unsaturated ester copolymer is made of a metal embossing roll 21 such as stainless steel having a fine concavo-convex pattern, and It is inserted between the rubber-made pressing rolls 22 such as silicone rubber and chloroprene rubber which are arranged to face each other. Then while conveying the film 30 in the direction of the arrow, that push heating between the embossing roll 21 and rubber press roll 22. At this time, the fine uneven pattern of the embossing roll 21 is transferred to the film 30. The temperature of the embossing roll 21 varies depending on the composition of the composition of the film 30, but is preferably 20 to 40 ° C., particularly preferably 20 to 30 ° C. Subsequently, the film 30 passes through the first guide roll 23a and is cooled while being transported under a predetermined tension by the second guide roll 23b and the third guide roll 23c. can get. Usually, the obtained film 40 for laminated body formation is wound up in roll shape (not shown), and is stored until it is used.

  The film 30 can be obtained, for example, by putting a composition containing an ethylene-unsaturated ester copolymer and a crosslinking agent into a mixing roll or the like, melt-kneading, and then forming the film. A conventionally known molding method can be used as the molding method. For example, a calendar molding method, an extrusion molding method, an injection molding method, or a heating press method can be used. The calendering method is particularly useful because a film having a uniform thickness can be produced at high speed. The calender molding method is a method in which a composition is mixed by melt kneading or the like, then placed in a heating roll and rolled to form a film. Although the mixing temperature of a composition changes with mixing | blendings, it is preferable to carry out by heat-kneading at the temperature of 40-90 degreeC, especially 60-80 degreeC, for example. Moreover, about the temperature of a heating roll, when a crosslinking agent is included, it is preferable to set it as the temperature which a crosslinking agent does not react or hardly reacts. For example, it is preferable to set it as 40-90 degreeC, especially 50-80 degreeC. The film 30 may be formed by an apparatus that continuously performs the film forming and embossing process, or may be performed by an apparatus that forms only the film 30 in advance.

Explaining in more detail the embossing step by the embossing roll 21, as shown in FIG. 1B, the uneven pattern 24 of the embossing roll 21 is pressed against the embossing surface 31 of the film 30, and the rubber pressing roll 22. Due to this elasticity, the concavo-convex pattern 24 is sufficiently transferred to the embossed surface 31. At this time, the non-embossed surface 32 of the film 30 is pressed against the roll surface 25 of the rubber pressing roll 22. Since the material of the rubber pressure roll 22 is rubber, generally, the roll surface 25 is not as smooth as the metal surface, and has fine irregularities. Therefore, the non-embossed surface 32 of the film 30 partially transfers the fine unevenness of the roll surface 25 of the rubber pressure roll 22, and the non-embossed surface 32 is good due to the transferred fine unevenness. You may not get a tack.

  In the present invention, the arithmetic average roughness Ra of the roll surface 25 is 0.5 to 1.5 [mu] m, preferably 1.0 to 1.5 [mu] m, and the rubber pressing roll 22 with respect to the embossed surface 31 of the film 30 is used. Even if embossing is sufficiently performed and fine irregularities on the roll surface 25 of the rubber pressing roll 22 are transferred to the non-embossed surface 32, the non-embossed surface 32 having a good tack can be obtained. When the arithmetic average roughness Ra of the roll surface 25 of the rubber pressure roll 22 is smaller than 0.5 μm, the surface of the rubber pressure roll 22 becomes too smooth and the tack of the non-embossed surface 32 becomes too high. In that case, it becomes difficult to correct the position when the films 30 are laminated. Furthermore, the embossing on the embossed surface 31 may be insufficient, and when the arithmetic average roughness Ra of the roll surface 25 is larger than 1.5 μm, the tack of the non-embossed surface 32 is lowered.

  In the present invention, the arithmetic average roughness Ra of the rubber pressing roll surface is a value measured by a method based on JIS-B0601 (1994). That is, a predetermined length is extracted from the roughness curve in the direction of the average line, and the absolute values of deviations from the average line of the extracted portion to the measurement curve are summed and averaged.

  Further, in the present invention, “good tack” means that the non-embossed surface is brought into contact with a glass plate, a load of 500 g is applied for 90 seconds, and then peeled off at a speed of 300 mm / min (tack meter (MODEL: (Measured with DPX-SOT (manufactured by Imada)) is preferably 0.4 N or more.

  In the present invention, by controlling the arithmetic average roughness Ra of the roll surface 25 of the rubber pressing roll 22, a good tack of the non-embossed surface 32 of the film 30 can be obtained. There is no limit. Generally, the press pressure of the embossing roll 21 is 0.1 to 3.0 MPa. In order to obtain a non-embossed surface having better tack, the press pressure of the embossing roll 21 is preferably 0.1 to 1.0 MPa. When the pressing pressure of the embossing roll 21 is smaller than 0.1 MPa, the transferability of the embossing with respect to the embossing surface 31 of the film 30 is inferior.

  As described above, the laminate-forming film 40 obtained by the present invention may have fine irregularities formed on the non-embossed surface by the roll surface 25 of the rubber pressing roll 22 as a result. The surface state of the non-embossed surface of the film 40 for forming a laminated body is not limited to the arithmetic average roughness Ra of the roll surface 25 of the rubber pressing roll 22, and the film is pressed when the embossing roll 21 or the film 30 is conveyed. Also affected by the tension applied to 30. In order to obtain a non-embossed surface having a better tack, the average interval Sm between the irregularities is preferably 600 μm or more, particularly preferably 600 to 1600 μm. The arithmetic average roughness Ra of the surface of the non-embossed surface is preferably 2.2 μm or less, particularly preferably 1.0 to 2.2 μm.

  In addition, in this invention, arithmetic mean roughness Ra of the surface of a non-embossed surface is the value measured by the method based on JIS-B0601 (1994) similarly to the case of said rubber press roll surface. Moreover, the average interval Sm of unevenness | corrugation is the value measured by the method based on JIS-B0601 (1994). That is, a predetermined length is extracted from the roughness curve in the direction of the average line, and the sum of the lengths of the average lines corresponding to one peak of the extracted portion and one valley adjacent thereto is obtained. The average value.

  In the present invention, the fine concavo-convex pattern 24 of the embossing roll 21 is particularly limited as long as embossing capable of preventing blocking during storage and improving deaeration during production can be imparted to the embossed surface of the laminate-forming film 40. There is no. For example, the convex portions in the concavo-convex shape can be provided as a circular shape, a semicircular shape, or a polygonal shape with a required interval, or the convex portions can be provided as a stripe shape or a mesh shape. In particular, since the manufacturing is easy, it is preferable that the convex portion has a concave and convex shape provided in a stripe shape. Moreover, arithmetic mean roughness Ra of the surface of an embossing roll is 3-50 micrometers normally.

  The average thickness of the laminate-forming film 40 varies depending on the application, but is generally preferably 50 μm to 2 mm, particularly preferably 100 μm to 1.5 mm.

  The ethylene-unsaturated ester copolymer used in the present invention is not particularly limited and can be used depending on the application. For example, as an unsaturated ester monomer of an ethylene-unsaturated ester copolymer, vinyl acetate, vinyl ester such as vinyl propionate, methyl acrylate, ethyl acrylate, isobutyl acrylate, n-butyl acrylate, And unsaturated carboxylic acid esters such as isooctyl acrylate, methyl methacrylate, isobutyl methacrylate, dimethyl maleate, and diethyl maleate.

  Specific examples of the ethylene-unsaturated ester copolymer include ethylene-vinyl ester copolymers such as ethylene-vinyl acetate copolymer (EVA), ethylene ethyl acrylate copolymer (EEA), and ethylene-methyl methacrylate. And ethylene-unsaturated carboxylic acid ester copolymers such as copolymers. Among these, an ethylene-vinyl acetate copolymer is preferable because a laminate-forming film having excellent adhesion and transparency can be produced.

  The vinyl acetate content of the ethylene-vinyl acetate copolymer is not particularly limited and can be selected depending on the application. 20-35 mass parts is preferable with respect to 100 mass parts of ethylene-vinyl acetate copolymers, 20-30 mass parts is more preferable, and 24-28 mass parts is especially preferable. The lower the content of EVA in vinyl acetate units, the harder the EVA composition. On the other hand, if the content of vinyl acetate is less than 20 parts by mass, the transparency of the EVA composition may decrease. Moreover, when it exceeds 35 mass parts, when a resin layer is formed with an EVA composition, hardness may become inadequate.

  In the present invention, the composition constituting the film can be prepared by adding a crosslinking agent, a crosslinking aid, an adhesion improver, a plasticizer and the like to the ethylene-unsaturated ester copolymer as necessary. .

As the crosslinking agent, an organic peroxide that decomposes at a temperature of 100 ° C. or higher to generate radicals can be used. The organic peroxide is generally selected in consideration of the film formation temperature, the adjustment conditions of the composition, the curing temperature, the heat resistance of the adherend, and the storage stability. In particular, the one having a decomposition temperature of 70 ° C. or more with a half-life of 10 hours is preferable. As the organic peroxide, from the viewpoint of the processing temperature and storage stability of the resin, for example,
1,4-bis (t-butylperoxycarbonyloxy) hexane, 1,5-bis (t-butylperoxycarbonyloxy) hexane, 1,6-bis (t-butylperoxycarbonyloxy) hexane, 2,2-dimethyl Compounds having a bifunctional peroxymonocarbonate structure such as -1,3-bis (t-butylperoxycarbonyloxy) propane, benzoyl peroxide, 2,5-dimethylhexyl-2,5-bisperoxybenzoate, etc. Benzoyl peroxide curing agent, tert-butylperoxy-2-ethylhexyl monocarbonate, 1,1-bis (tert-hexylperoxy) -3,3,5-trimethylcyclohexane, tert-hexylperoxypivalate, tert -Butylperoxypiva 3,5,5-trimethylhexanoyl peroxide, di-n-octanoyl peroxide, lauroyl peroxide, stearoyl peroxide, 1,1,3,3-tetramethylbutylperoxy-2-ethylhexa Noate, succinic acid peroxide, 2,5-dimethyl-2,5-di (2-ethylhexanoylperoxy) hexane, 1-cyclohexyl-1-methylethylperoxy-2-ethylhexanoate, tert -Hexylperoxy-2-ethylhexanoate, 4-methylbenzoyl peroxide, tert-butylperoxy-2-ethylhexanoate, m-toluoyl + benzoyl peroxide, benzoyl peroxide, 1,1-bis ( tert-butylperoxy) -2-me Lucyclohexanate, 1,1-bis (tert-hexylperoxy) -3,3,5-trimethylcyclohexanate, 1,1-bis (tert-hexylperoxy) cyclohexanate, 1,1-bis (Tert-butylperoxy) cyclohexanate, 2,2-bis (4,4-di-tert-butylperoxycyclohexyl) propane, 1,1-bis (tert-butylperoxy) cyclododecane, tert-hexyl Peroxyisopropyl monocarbonate, tert-butylperoxymaleic acid, tert-butylperoxy-3,3,5-trimethylhexanoate, tert-butylperoxylaurate, 2,5-dimethyl-2,5- Di (methylbenzoylperoxy) hexane, tert-butylper Examples include oxyisopropyl monocarbonate, tert-hexylperoxybenzoate, 2,5-di-methyl-2,5-di (benzoylperoxy) hexane, and the like. These crosslinking agents may be used alone or in combination of two or more. The amount of the crosslinking agent used is preferably 0.05 to 5 parts by mass, more preferably 0.1 to 3 parts by mass, and particularly preferably 0.5 to 2 parts by mass with respect to 100 parts by mass of the ethylene-unsaturated ester copolymer. 5 parts by mass.

  The crosslinking aid can improve the gel fraction of the ethylene-unsaturated ester copolymer and improve the adhesiveness and durability of the laminate-forming film. Examples of the crosslinking aid (compound having a radical polymerizable group as a functional group) include trifunctional crosslinking aids such as triallyl cyanurate and triallyl isocyanurate, and (meth) acrylic esters (eg, NK ester). And monofunctional or bifunctional crosslinking aids. Of these, triallyl cyanurate and triallyl isocyanurate are preferable, and triallyl isocyanurate is particularly preferable. These crosslinking assistants are generally used in an amount of 10 parts by mass or less, preferably 0.1 to 5 parts by mass with respect to 100 parts by mass of the ethylene vinyl acetate copolymer.

  As the adhesion improver, a silane coupling agent can be used. Examples of silane coupling agents include γ-chloropropylmethoxysilane, vinylethoxysilane, vinyltris (β-methoxyethoxy) silane, γ-methacryloxypropyltrimethoxysilane, vinyltriacetoxysilane, γ-glycidoxypropyltrimethoxy. Silane, γ-glycidoxypropyltriethoxysilane, β- (3,4-epoxycyclohexyl) ethyltrimethoxysilane, vinyltrichlorosilane, γ-mercaptopropyltrimethoxysilane, γ-aminopropyltriethoxysilane, N-β Mention may be made of-(aminoethyl) -γ-aminopropyltrimethoxysilane. These silane coupling agents may be used alone or in combination of two or more. Moreover, it is preferable that content of the said adhesive improvement agent is 5 mass parts or less with respect to 100 mass parts of ethylene-unsaturated ester copolymers.

  Examples of plasticizers include phosphites such as trisisodecyl phosphite and trisnonylphenyl phosphite and phosphorus-containing compounds such as phosphate esters, adipic acid ether esters, trimellitate n-octyl, dioctyl phthalate, dihexyl adipate, sebacic acid Esters of polybasic acids such as dibutyl, 2,2,4-trimethyl-1,3-pentanediol disobutyrate, triethylene glycol-di-2-ethylbutyrate, tetraethylene glycol diheptanoate, triethylene glycol Polyesters such as dipelargonate, epoxidized fatty acid alkyl esters and the like can be used.

  Moreover, you may use the other additive of said material for the composition in this invention by the use of the film for laminated body formation. For example, when used as an interlayer film for laminated glass or a sealing film for solar cells, various physical properties (such as mechanical properties, optical properties such as adhesion, transparency, heat resistance, light resistance, crosslinking speed, etc.) Alternatively, various additives such as an acryloxy group-containing compound, a methacryloxy group-containing compound, an epoxy group-containing compound, an ultraviolet absorber, a light stabilizer, and / or an anti-aging agent may be added as necessary for adjustment. .

  The film for forming a laminate obtained by the present invention is embossed on one side, blocking resistance during storage, deaeration during production is ensured, and the non-embossed surface has a good tack. Therefore, it can be preferably used as an interlayer film for laminated glass or a sealing film for solar cell, which requires precise positioning during lamination.

  When used as an interlayer film for laminated glass, the laminated glass film (intermediate film) produced according to the present invention is usually interposed between two transparent substrates to produce a laminated glass by bonding and integrating them. To do. As the transparent substrate, for example, a plastic film may be used in addition to a glass plate such as a silicate glass, an inorganic glass plate, and a non-colored transparent glass plate. Examples of the plastic film include a polyethylene terephthalate (PET) film, a polyethylene aphthalate (PEN) film, and a polyethylene butyrate film, and a PET film is preferred. The thickness of the transparent substrate is generally about 0.05 to 20 mm.

  Laminated glass is usually produced by sandwiching and laminating an interlayer film between two transparent substrates, degassing the stack under reduced pressure, and pressing it under heating (high temperature laminating step). It is carried out by cross-linking and curing the ethylene-unsaturated ester copolymer contained and bonding and integrating the layers. In the case of crosslinking and curing, the laminate is generally subjected to a heat treatment at 100 to 150 ° C., particularly around 130 ° C., for 10 to 120 minutes, preferably 10 to 60 minutes. The cross-linking curing may be performed after pre-bonding at a temperature of, for example, 80 to 120 ° C. The heat treatment is particularly preferably, for example, at 130 ° C. for 10 to 30 minutes (atmospheric temperature). Moreover, it is preferable to perform the said heat processing, applying the press pressure of 0-800 KPa to a laminated body. Although cooling of the laminated body after crosslinking is generally performed at room temperature, the faster the cooling, the better.

  Moreover, when using for the sealing film for solar cells, the laminated body formation film (sealing film) manufactured by this invention is usually interposed between the surface side transparent protective member and the back surface side protective member. Then, the cells for solar cells are sealed by crosslinking and integrated to produce a solar cell. In order to sufficiently seal the solar cell, the front side transparent protective member, the front side sealing film, the solar cell, the back side sealing film and the back side protective member are laminated in that order, After pre-pressing under reduced pressure and degassing the air remaining in each layer, the sealing film may be crosslinked and cured by heating and pressurization.

  Here, the side of the solar cell irradiated with light (light receiving surface side) is referred to as “front surface side”, and the side opposite to the light receiving surface of the solar battery cell is referred to as “back surface side”.

  The surface-side transparent protective member used for solar cells is usually preferably a glass substrate such as silicate glass. As for the thickness of a glass substrate, 0.1-10 mm is common, and 0.3-5 mm is preferable. The glass substrate may generally be chemically or thermally strengthened. The back side protective member is a plastic film such as polyethylene terephthalate (PET). In consideration of heat resistance and moist heat resistance, a fluorinated polyethylene film, particularly a fluorinated polyethylene film / Al / fluorinated polyethylene film is used in this order. A film laminated with is preferable.

For example, the heating and pressurization may be performed by using a vacuum laminator to heat the laminated body at a temperature of 135 to 180 ° C., further 140 to 180 ° C., particularly 155 to 180 ° C., a degassing time of 0.1 to 5 minutes, and a press pressure of 0.1 to What is necessary is just to heat-press in 1.5 kg / cm < ² > and press time for 5 to 15 minutes. At the time of this heating and pressurizing, the EVA contained in the front side sealing film and the rear side sealing film is cross-linked, whereby the front side transparent protective member, the rear side, through the front side sealing film and the rear side sealing film. The solar cell can be sealed by integrating the transparent member and the solar cell.

Hereinafter, the present invention will be described with reference to examples.
(Preparation of laminate-forming film)
(Examples 1-4, Comparative Examples 1-3)
The following formulation:
EVA (content of vinyl acetate with respect to 100 parts by mass of EVA; 26 parts by mass); 100 parts by mass crosslinking agent (2,5-dimethyl-2,5-di (t-butylperoxy) hexane); 1 part by mass crosslinking aid (Triallyl isocyanurate); 2 parts by mass additive (γ-methacryloxypropyltrimethoxysilane); 0.5 part by mass is supplied to a roll mill and kneaded at 70 ° C. to prepare an EVA composition at 70 ° C. Then, it was calendered to obtain a film. Subsequently, with respect to the embossed surface of the film, an embossed roll having a fine concavo-convex shape pattern (arithmetic surface roughness Ra; 10 μm) having a striped shape, and the arithmetic average roughness of the roll surface shown in Table 1 Embossing was applied at a pressing pressure of 0.6 MPa of the embossing roll and a roll temperature of 30 ° C. using a rubber pressing roll having a thickness Ra. Then, it cooled, conveying a film with a guide roll, wound up in roll shape, and obtained the film (thickness 0.6mm) for laminated body formation.

(Evaluation method)
(1) Measurement of tack The non-embossed surface of each laminate-forming film produced above was brought into contact with a glass plate, and after applying a load of 500 g for 90 seconds, the adhesion when peeled off at a speed of 300 mm / min. It measured with the tack meter (MODEL: DPX-SOT (made by Imada)). Adhesion was 0.4N or more and passed.
(2) Emboss transferability The state of the embossed surface of each laminate-forming film prepared above is visually observed, ◯ when the emboss is clearly formed, △ when there are a few unclear parts, When the unclear part was conspicuous, it evaluated as x. △ or more was accepted.
(3) Measurement of arithmetic average roughness Ra of surface and average interval Sm of unevenness Measured by a method based on JIS-B0601 (1994) using a surface roughness meter (Suronic 3+ (manufactured by Rank Taylor Hobson)). did.

(Evaluation results)
Table 1 shows the results of the above evaluations. In Examples 1 to 4, the arithmetic average roughness Ra of the surface of the rubber pressing roll was 0.5 to 1.5 μm, and the pressing pressure of the embossing roll was 0.6 MPa. The non-embossed surface tack was 0.4 to 1.5 N, which was acceptable. Moreover, the emboss transferability of the embossed surface was also acceptable. In these cases, the average unevenness Sm of the non-embossed surface of the film was 600 to 1600 μm, and the arithmetic average roughness Ra of the surface was 1.2 to 2.2 μm. On the other hand, when the arithmetic average roughness Ra of the surface of the rubber pressing roll was 1.8 to 2.3 μm, the embossed transferability of the embossed surface was good, but the resulting film was not embossed. The tack of the surface was 0.3N, which was not acceptable.

  By the above, when embossing of the film for forming a laminate is performed, the embossed surface of the film is sufficiently embossed by setting the arithmetic average roughness Ra of the surface of the rubber pressing roll to 0.5 to 1.5 μm. It was recognized that a non-embossed surface having good tack can be obtained while performing transfer.

  In addition, this invention is not limited to the structure and Example of said embodiment, A various deformation | transformation is possible within the range of the summary of invention.

  By using the ethylene-unsaturated ester copolymer film for forming a laminate obtained by the production method of the present invention as an intermediate film for laminated glass or a sealing film for solar cell, high yield laminated glass or A solar cell can be manufactured.

5 Intermediate glass for laminated glass 7A, 7B Glass plate 11 Front side transparent protective member 12 Back side protective member 13A Front side sealing film 13B Back side sealing film 14 Solar cell 21 Embossing roll 22 Rubber pressure roll 23a First guide Roll 23b Second guide roll 23c Third guide roll 24 Concave and convex pattern 25 Roll surface 30 Film 31 Embossed surface 32 Non-embossed surface 40 Laminate forming film

Claims (6)

A film comprising a composition containing an ethylene-unsaturated ester copolymer is inserted between an embossing roll having a fine concavo-convex pattern and a rubber pressing roll disposed opposite to the embossing roll, and the film is embossed. In the method for producing a film for forming a laminate, including a step of transferring an emboss only to one surface of the film by pressing a roll ,
The manufacturing method characterized by arithmetic mean roughness Ra of the surface of the said rubber | gum press roll being 0.5-1.5 micrometers.   The manufacturing method according to claim 1, wherein fine irregularities are formed on a surface opposite to the surface to which the emboss is transferred of the laminate forming film, and an average interval Sm between the irregularities is 600 to 1600 μm.   The method according to claim 1 or 2, wherein the laminate-forming film has an arithmetic average roughness Ra of 1.0 to 2.2 µm on the surface opposite to the surface to which the emboss is transferred.   The manufacturing method according to any one of claims 1 to 3, wherein the ethylene-unsaturated ester copolymer is an ethylene-vinyl acetate copolymer.   The method according to claim 4, wherein the ethylene-vinyl acetate copolymer has a vinyl acetate repeating unit content of 20 to 35 parts by mass with respect to 100 parts by mass of the ethylene-vinyl acetate copolymer.   The manufacturing method according to claim 1, wherein the laminate-forming film is an interlayer film for laminated glass or a sealing film for solar cells.

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