Ethylene / α-olefin / non-conjugated polyene copolymer, pellet, resin composition, uncrosslinked sheet, crosslinked body, sealing material, solar cell module, and method for producing solar cell module

Abstract

One embodiment of the present invention relates to an ethylene / α-olefin / non-conjugated polyene copolymer. The copolymer has a structural unit derived from ethylene (A1), a structural unit derived from an α-olefin (A2) having 4 or more carbon atoms, and a structural unit derived from a non-conjugated polyene (A3) containing, in each molecule, a total of two or more partial structures of at least one type selected from the group consisting of general formulae (I) and (II). When the total of the structural units derived from (A1), (A2), and (A3) is taken as 100 mol%, the content ratio of the structural unit derived from ethylene (A1) is 75.0-95.0 mol%, the content ratio of the structural unit derived from the α-olefin (A2) is 4.9-24.9 mol%, and the content ratio of the structural unit derived from the non-conjugated polyene (A3) is 0.1-1.0 mol%.

Description

Ethylene-α-olefin-non-conjugated polyene copolymer, pellets, resin composition, uncrosslinked sheet, crosslinked body, encapsulant, solar cell module, and method for manufacturing solar cell module.

[0001] The present invention relates to ethylene-α-olefin-non-conjugated polyene copolymer, pellets, resin compositions, uncrosslinked sheets, crosslinked bodies, encapsulants, solar cell modules, and methods for manufacturing solar cell modules.

[0002] Amidst worsening global environmental and energy problems, solar cells are attracting attention as a clean and inexhaustible means of energy generation. When solar cells are used outdoors, such as on the roofs of buildings, they are generally used in the form of solar cell modules.

[0003] Solar cell modules are generally manufactured using the following procedure. First, crystalline solar cell elements (sometimes referred to as power generation elements or cells) formed from polycrystalline silicon, monocrystalline silicon, etc., or thin-film solar cell elements obtained by forming a very thin film of several micrometers on a substrate such as glass using amorphous silicon or crystalline silicon are manufactured. Next, when obtaining a crystalline solar cell module using an encapsulating sheet (uncrosslinked sheet), the layers are stacked in the following order: "solar cell module protective sheet (surface protective sheet) / encapsulating sheet / crystalline solar cell element / encapsulating sheet / solar cell module protective sheet (back protective sheet)". When obtaining a thin-film solar cell module using the aforementioned encapsulating sheet, the layers are stacked in the following order: "thin-film solar cell element / encapsulating sheet / solar cell module protective sheet (back protective sheet)". After that, these stacked structures are assembled into modules using a lamination method, which involves vacuum suction and heat compression. Solar cell modules manufactured using this method have weather resistance and are therefore suitable for outdoor use, such as on the roofs of buildings.

[0004] In recent years, olefin-based elastomers have attracted attention as materials for sealing sheets before crosslinking, due to their excellent transparency, crosslinkability, and electrical insulation properties after crosslinking, which are used as sealing materials. For example, Patent Documents 1 and 2 disclose sealing materials containing ethylene-α-olefin-non-conjugated polyene copolymers that are excellent in various properties such as transparency, flexibility, adhesion, heat resistance, appearance, crosslinkability, electrical properties, and calendering properties.

[0005] International Publication No. 2012 / 066783, International Publication No. 2012 / 070245

[0006] To further improve the mechanical strength and heat resistance of crosslinked materials after crosslinking, there is a demand for olefin-based elastomers with higher crosslinking capabilities. Furthermore, sheet sticking can occur after manufacturing, potentially reducing workability and productivity. Therefore, to suppress sheet sticking, low peel strength between sheets (hereinafter also referred to as "sheet blocking resistance") is required.

[0007] The object of the present invention is to provide an ethylene-α-olefin-non-conjugated polyene copolymer, pellets containing the copolymer, a resin composition containing the copolymer, a sheet containing the composition, a crosslinked body containing the resin composition or the sheet, a encapsulant containing the crosslinked body, a solar cell module equipped with the encapsulant, and a method for manufacturing the solar cell module, which can produce pellets with high crosslinkability and excellent sheet blocking resistance of the molded sheet.

[0008] As a result of their investigations to solve the above problems, the present inventors have found that the above problems can be solved by an ethylene-α-olefin-non-conjugated polyene copolymer that satisfies predetermined requirements, and have completed the present invention. That is, according to the present invention, for example, the ethylene-α-olefin-non-conjugated polyene copolymers shown in [1] to

[24] below are provided.

[0009] [1] Ethylene-α-olefin-non-conjugated polyene copolymer (A) having structural units derived from ethylene [A1], structural units derived from α-olefin [A2] having 4 or more carbon atoms, and structural units derived from non-conjugated polyene [A3] containing a total of two or more substructures selected from the group consisting of the following general formulas (I) and (II) in one molecule, and satisfying the following requirements (a1) to (a3): (a1) The content of structural units derived from ethylene [A1] is 75.0 to 95.0 mol%, with the total of structural units derived from [A1], [A2] and [A3] being 100 mol%; (a2) The content of structural units derived from α-olefin [A2] is 4.9 to 24.9 mol%, with the total of structural units derived from [A1], [A2] and [A3] being 100 mol%; (a3) The content of structural units derived from non-conjugated polyene [A3] is 0.1 to 1.0 mol%, with the total of structural units derived from [A1], [A2], and [A3] being 100 mol%.

[0010]

[0011] [2] The ethylene-α-olefin-non-conjugated polyene copolymer (A) according to [1], wherein the α-olefin [A2] having 4 or more carbon atoms is 1-butene. [3] The ethylene-α-olefin-non-conjugated polyene copolymer (A) according to [1], wherein the non-conjugated polyene [A3] contains 5-vinyl-2-norbornene. [4] The ethylene-α-olefin-non-conjugated polyene copolymer (A) according to [1], wherein the α-olefin [A2] having 4 or more carbon atoms is 1-butene, and the non-conjugated polyene [A3] contains 5-vinyl-2-norbornene. [5] The ethylene-α-olefin-non-conjugated polyene copolymer (A) according to any one of [1] to [3], wherein the molar ratio [[A1] / [A3]] of structural units derived from ethylene [A1] to structural units derived from non-conjugated polyene [A3] is 100 to 1200. [6] The ethylene-α-olefin-non-conjugated polyene copolymer (A) according to [1], wherein the α-olefin [A2] having 4 or more carbon atoms is 1-butene, the non-conjugated polyene [A3] contains 5-vinyl-2-norbornene, and the molar ratio [[A1] / [A3]] of structural units derived from ethylene [A1] to structural units derived from non-conjugated polyene [A3] is 100 to 1200.

[0012] [7] Furthermore, an ethylene-α-olefin-non-conjugated polyene copolymer (A) described in any of [1] to [6] that satisfies the following requirement (a4): (a4) The melt flow rate measured at 190°C and a 2.16 kg load in accordance with ASTM D1238 is 3 to 20 g / 10 min. [8] Furthermore, an ethylene-α-olefin-non-conjugated polyene copolymer (A) described in any of [1] to [7] that satisfies the following requirement (a5): (a5) MFR １０ / MFR ２ However, it is in the range of 5.0 to 8.0 (MFR １０ This is the melt flow rate measured at 190°C and a 10 kg load in accordance with ASTM D1238, and MFR ２is a melt flow rate measured at 190°C under a load of 2.16 kg in accordance with ASTM D1238.). [9] The ethylene / α-olefin / non-conjugated polyene copolymer (A) according to any one of [1] to [8], which further satisfies the following requirement (a6): (a6) The glass transition temperature (Tg) measured by differential scanning calorimetry (DSC) is -50°C or lower.

[10] The α-olefin having 4 or more carbon atoms [A2] is 1-butene, the non-conjugated polyene [A3] contains 5-vinyl-2-norbornene, and the molar ratio of the structural unit derived from ethylene [A1] to the structural unit derived from the non-conjugated polyene [A3] [[A1] / [A3]] is from 100 to 1200, and the melt flow rate measured at 190°C under a load of 2.16 kg in accordance with ASTM D1238 is from 6.0 to 18 g / 10 min. The ethylene / α-olefin / non-conjugated polyene copolymer (A) according to any one of [1] to [9].

[0013]

[11] A pellet comprising the ethylene / α-olefin / non-conjugated polyene copolymer (A) according to any one of [1] to

[10] .

[12] A resin composition comprising the ethylene / α-olefin / non-conjugated polyene copolymer (A) according to any one of [1] to

[10] , a hydrosilyl group-containing compound (D), and a platinum-based catalyst (E).

[13] The resin composition according to

[12] , wherein the hydrosilyl group-containing compound (D) is an organohydrogenpolysiloxane represented by the following general formula (d).

[0014] (In formula (d), n and p are each independently 0 or a positive integer, m is an integer of 1 to 20, and the sum of n, m and p is 5 to 50. A plurality of R １ and R ２ are each independently a monovalent alkyl group, R ａ is an aralkyl group, two R groups are each independently selected from a hydrogen atom, R １ , R ２ , and R ａ is a group selected from the group consisting of, -[O-Si(R １ )(R ａ )]-, -[O-Si(R １)H]- and -[O-Si(R １ ) (Caution ２ The structural units represented by )- may be arranged in a block-like manner or randomly. However, when n=1, at least one of the two R atoms is a hydrogen atom, and when n=0, both R atoms are hydrogen atoms.

[0015]

[14] The resin composition according to

[12] or

[13] , comprising 0.1 to 100 parts by mass of the hydrosilyl group-containing compound (D) per 100 parts by mass of the ethylene-α-olefin-non-conjugated polyene copolymer (A), and comprising 0.000001 to 5 parts by mass of the platinum-based catalyst (E) per 100 parts by mass of the ethylene-α-olefin-non-conjugated polyene copolymer (A).

[15] The resin composition according to any one of

[12] to

[14] , further comprising a reaction inhibitor (F), comprising 0.001 to 5 parts by mass of the reaction inhibitor (F) per 100 parts by mass of the ethylene-α-olefin-non-conjugated polyene copolymer (A).

[16] The resin composition according to any one of

[12] to

[15] , further comprising an adhesion promoter (G) which is a silane-modified resin, wherein the adhesion promoter (G) is present in an amount of 10 to 40 parts by mass per 100 parts by mass of the ethylene-α-olefin-non-conjugated polyene copolymer (A).

[0016]

[17] An uncrosslinked sheet comprising the resin composition described in any of

[12] to

[16] .

[18] The uncrosslinked sheet described in

[17] for use as a encapsulant.

[19] A crosslinked body obtained by crosslinking the resin composition described in any of

[12] to

[16] or the uncrosslinked sheet described in

[17] .

[20] An encapsulant comprising the crosslinked body described in

[19] .

[21] The encapsulant described in

[20] for use as a solar cell.

[0017]

[22] A solar cell module comprising a front-side transparent protective member, a back-side protective member, a solar cell element, and a sealing layer containing the sealing material described in

[20] or

[21] , wherein the sealing layer seals the solar cell element between the front-side transparent protective member and the back-side protective member.

[23] The solar cell module according to

[22] , wherein the solar cell element comprises at least one type of perovskite compound.

[24] A method for manufacturing a solar cell module, comprising the steps of (i) stacking a front-side transparent protective member, an uncrosslinked sheet described in

[17] , a solar cell element, and a back-side protective member in this order to form a laminate, and (ii) pressing and heating the laminate to integrate it, wherein the heating temperature in step (ii) is 130°C or less.

[0018] The crosslinked material obtained using the ethylene-α-olefin-non-conjugated polyene copolymer of the present invention exhibits high crosslinkability, and the molded sheet further exhibits excellent resistance to sheet blocking.

[0019] The present invention will now be described in detail. In this specification, the terms "(co)polymer" and "polymer" are used to encompass homopolymers and copolymers. In this specification, the expression "x to y" (where x and y are numerical values, but x ≠ y) which indicates a numerical range, means "x or greater and y or less" when x < y, and "x or less and y or greater" when x > y, unless otherwise specified. In addition, the units indicated before and after the "~" indicating a numerical range refer to the same units unless otherwise specified.

[0020] In this specification, "structural unit derived from ethylene" means the structural unit corresponding to ethylene, i.e., -CH ２ -CH ２ This refers to the structural unit represented by -. The same interpretation applies to "structural units derived from α-olefins," which are the structural units corresponding to α-olefins, namely -CH ２This refers to a structural unit represented by -CRR'- (where R and R' are independently hydrogen or alkyl groups). Furthermore, "structural unit derived from a non-conjugated polyene" refers to a structural unit corresponding to a non-conjugated polyene, that is, a structural unit having one or more bonds formed by the cleavage of one or more π bonds constituting a double bond in the non-conjugated polyene.

[0021] In this specification, a combination of two or more preferred embodiments is a more preferred embodiment. In numerical ranges described stepwise in this specification, the upper or lower limit of one numerical range may be replaced with the upper or lower limit of another numerical range described stepwise. Also, in numerical ranges described in this specification, the upper or lower limit of that numerical range may be replaced with the values ​​shown in the examples.

[0022] In this specification, unless otherwise specified, each constituent unit in a polymer may be present as a single entity or as two or more entities. If multiple entities of each constituent unit are present in a polymer, the content or proportion of each constituent unit means the total content or proportion of each entity present in the polymer, unless otherwise specified. In this specification, unless otherwise specified, each component may be present as a single entity or as two or more entities. If multiple entities corresponding to each component are present in a composition, the content or proportion of each component means the total content or proportion of each entity present in the composition, unless otherwise specified.

[0023] In this specification, "%" indicating the amount or percentage of a component is based on mass unless otherwise specified. In this specification, "layer" includes cases where the layer is formed throughout the entire region when the region in which the layer exists is observed, as well as cases where it is formed only on a part of the region. In this specification, "process" includes not only processes that are independent of other processes, but also processes that cannot be clearly distinguished from other processes, provided that the purpose of the process is achieved.

[0024] Ethylene-α-olefin-non-conjugated polyene copolymer (A) The ethylene-α-olefin-non-conjugated polyene copolymer (A) (hereinafter also referred to as "copolymer (A)") according to one embodiment of the present invention includes structural units derived from ethylene [A1], structural units derived from α-olefin [A2] having 4 or more carbon atoms (hereinafter also referred to as "α-olefin [A2]"), and structural units derived from non-conjugated polyene [A3]. Here, the non-conjugated polyene [A3] contains a total of two or more substructures selected from the group consisting of the following general formulas (I) and (II) in one molecule.

[0025]

[0026] Furthermore, the copolymer (A) of the present invention satisfies the following requirements (a1) to (a3): (a1) The content of structural units derived from ethylene [A1] is 75.0 to 95.0 mol%, with the total of structural units derived from [A1], [A2], and [A3] being 100 mol%. (a2) The content of structural units derived from α-olefin [A2] is 4.9 to 24.9 mol%, with the total of structural units derived from [A1], [A2], and [A3] being 100 mol%. (a3) ​​The content of structural units derived from non-conjugated polyene [A3] is 0.1 to 1.0 mol%, with the total of structural units derived from [A1], [A2], and [A3] being 100 mol%.

[0027] α-olefin [A2] and non-conjugated polyene [A3] may be used individually or in combination of two or more. That is, the copolymer (A) comprises structural units derived from ethylene [A1], structural units derived from at least one type of α-olefin [A2], and structural units derived from at least one type of non-conjugated polyene [A3].

[0028] <α-olefin [A2]> The copolymer (A) of the present invention has structural units derived from α-olefin [A2] having 4 or more carbon atoms. Therefore, the glass transition temperature (Tg) is sufficiently low, and it exhibits excellent rubber elasticity at low temperatures. Examples of α-olefin [A2] having 4 or more carbon atoms that constitute the copolymer (A) of the present invention include linear α-olefins without side chains such as 1-butene, 1-pentene, 1-hexene, 1-heptene, 1-octene, 1-nonene, 1-decene, 1-dodecene, 1-nonadecene, and 1-eicosene; and branched α-olefins having side chains such as 4-methyl-1-pentene, 9-methyl-1-decene, 11-methyl-1-dodecene, and 12-ethyl-1-tetradecene. One type of α-olefin [A2] may be used, or two or more types may be used.

[0029] α-olefin [A2] is preferably an α-olefin having 4 to 20 carbon atoms, more preferably an α-olefin having 4 to 10 carbon atoms, and even more preferably comprises at least one selected from the group consisting of 1-butene, 1-hexene, and 1-octene, particularly preferably comprises 1-butene, and most preferably consists of 1-butene alone.

[0030] If α-olefin [A2] contains 1-butene, it may further contain α-olefins having 4 or more carbon atoms other than 1-butene. The α-olefins having 4 or more carbon atoms other than 1-butene may be 1-hexene or 1-octene.

[0031] <Non-conjugated polyene [A3]> The non-conjugated polyene [A3] constituting the copolymer (A) of the present invention contains a total of two or more substructures selected from the group consisting of the following general formulas (I) and (II) in one molecule.

[0032]

[0033] The non-conjugated polyene [A3] may have two or more substructures represented by the general formula (I), or two or more substructures represented by the general formula (II), or it may have one or more substructures represented by the general formula (I) and one or more substructures represented by the general formula (II).

[0034] Non-conjugated polyenes [A3] include, for example, linear non-conjugated dienes such as 1,4-hexadiene and 1,6-octadiene; cyclohexadiene, dicyclopentadiene, 5-vinyl-2-norbornene (VNB), norbornadiene, 5-(2-propenyl)-2-norbornene, 5-(3-butenyl)-2-norbornene, 5-(1-methyl-2-propenyl)-2-norbornene, 5-(4-pentenyl)-2-norbornene, 5-(5-hexenyl)-2-norbornene, 5-(1-methyl-4-pentenyl)-2-norbornene, 5-(2-ethyl-3-butenyl) Examples include cyclic non-conjugated dienes such as tenyl)-2-norbornene, 5-(6-heptenyl)-2-norbornene, 5-(3-methyl-5-hexenyl)-2-norbornene, 5-(3-ethyl-4-pentenyl)-2-norbornene, 5-(7-octenyl)-2-norbornene, 5-(2-methyl-6-heptenyl)-2-norbornene, 5-(1,2-dimethyl-5-hexenyl)-2-norbornene, and 5-(1,2,3-trimethyl-4-pentenyl)-2-norbornene; and trienes such as 1,3,7-octatriene and 1,4,9-decatriene.

[0035] The non-conjugated polyene [A3] may be one type or two or more types. The non-conjugated polyene [A3] is preferably a linear non-conjugated diene such as 1,4-hexadiene or a cyclic non-conjugated diene such as 5-vinyl-2-norbornene, more preferably a cyclic non-conjugated diene, even more preferably containing 5-vinyl-2-norbornene, and particularly preferably consisting only of 5-vinyl-2-norbornene. By using 5-vinyl-2-norbornene as the non-conjugated polyene [A3], crosslinking by the organic peroxide (B) or hydrosilyl group-containing compound (D) described later proceeds efficiently, and the mechanical properties of the crosslinked body and sealant described later tend to be good. The non-conjugated polyene [A3] is a non-conjugated polyene that, in addition to 5-vinyl-2-norbornene, contains a total of two or more substructures selected from the group consisting of general formulas (I) and (II) in its molecule, and may further contain non-conjugated polyenes other than 5-vinyl-2-norbornene (for example, cyclohexadiene).

[0036] <Non-conjugated polyene [A3']> The copolymer (A) of the present invention may further contain structural units derived from non-conjugated polyene [A3'], in addition to structural units derived from ethylene [A], structural units derived from α-olefin [A2], and structural units derived from non-conjugated polyene [A3].

[0037] Examples of non-conjugated polyenes [A3'] include 5-ethylidene-2-norbornene (ENB), 5-methylene-2-norbornene, 5-(2,3-dimethyl-3-butenyl)-2-norbornene, 5-(3,4-dimethyl-4-pentenyl)-2-norbornene, 5-(5-ethyl-5-hexenyl)-2-norbornene, and 5-(2-methyl-1-propenyl)-2-norbornene.

[0038] Among these, 5-ethylidene-2-norbornene (ENB) may be used because it is readily available, allows for easy control of the crosslinking rate during crosslinking with the organic peroxide (B) or hydrosilyl group-containing compound (D) described later, and makes it easy to obtain crosslinked bodies and encapsulants with good mechanical properties. The non-conjugated polyene [A3'] can be used alone or in combination of two or more types.

[0039] <Examples of Copolymer (A)> Preferred embodiments of copolymer (A) of the present invention include ethylene-1-butene-1,4-hexadiene copolymer, ethylene-1-pentene-1,4-hexadiene copolymer, ethylene-1-hexene-1,4-hexadiene copolymer, ethylene-1-heptene-1,4-hexadiene copolymer, ethylene-1-octene-1,4-hexadiene copolymer, ethylene-1-nonene-1,4-hexadiene copolymer, ethylene-1-decene-1,4-hexadiene copolymer, ethylene-1-butene-1-octene-1,4-hexadiene copolymer, ethylene-1-butene-VNB copolymer, ethylene-1-pentene-VNB copolymer, ethylene-1-hexene-VNB copolymer, ethylene Examples include n-1-heptene-VNB copolymer, ethylene-1-octene-VNB copolymer, ethylene-1-nonene-VNB copolymer, ethylene-1-decene-VNB copolymer, ethylene-1-butene-1-octene-VNB copolymer, ethylene-1-butene-ENB-VNB copolymer, ethylene-1-pentene-ENB-VNB copolymer, ethylene-1-hexene-ENB-VNB copolymer, ethylene-1-heptene-ENB-VNB copolymer, ethylene-1-octene-ENB-VNB copolymer, ethylene-1-nonene-ENB-VNB copolymer, ethylene-1-decene-ENB-VNB copolymer, and ethylene-1-butene-1-octene-ENB-VNB copolymer.

[0040] Among these, a more preferred embodiment of copolymer (A) is ethylene-1-butene-5-vinyl-2-norbornene (VNB) copolymer. The copolymer (A) constituting the resin composition of the present invention may be a single type or a combination of two or more types.

[0041] The copolymer (A) of the present invention satisfies the following requirements (a1) to (a3). <Requirement (a1)> The copolymer (A) of the present invention has a content ratio of structural units derived from ethylene [A1] of 75.0 to 95.0 mol%, where the total of the structural units of [A1], [A2], and [A3], i.e., the sum of structural units derived from ethylene [A1], structural units derived from α-olefin [A2], and structural units derived from non-conjugated polyene [A3] is 100 mol%.

[0042] The lower limit of the content of structural units derived from ethylene [A1] is preferably 78.0 mol%, more preferably 80.0 mol%, even more preferably 82.0 mol%, and particularly preferably 83.0 mol%, from the viewpoint of excellent sheet blocking resistance of the sheet and blocking resistance of the pellets containing copolymer (A) (hereinafter also referred to as "pellet handling properties"). The upper limit of the content of structural units derived from ethylene [A1] is preferably 92.0 mol%, more preferably 90.0 mol%, even more preferably 88.0 mol%, and particularly preferably 87.0 mol%, from the viewpoint of excellent crosslinking properties and flexibility. In other words, the content of structural units derived from ethylene [A1] is preferably 78.0 to 92.0 mol%, more preferably 80.0 to 90.0 mol%, even more preferably 82.0 to 88.0 mol%, and particularly preferably 83.0 to 87.0 mol%, from the viewpoint of excellent sheet blocking resistance and pellet handling properties, and excellent crosslinking properties and flexibility. The content of structural units derived from ethylene [A1] is, １ This can be measured using H-NMR. Specifically, it can be determined by the method described in the examples below. In addition, sheet blocking resistance and pellet handling properties can be evaluated by the method described in the examples below.

[0043] <Requirement (a2)> The copolymer (A) of the present invention has a content of structural units derived from α-olefin [A2] of 4.9 to 24.9 mol%, where 100 mol% is the sum of the structural units of [A1], [A2], and [A3], i.e., the sum of structural units derived from ethylene [A1], structural units derived from α-olefin [A2], and structural units derived from non-conjugated polyene [A3].

[0044] The lower limit of the content of structural units derived from α-olefin [A2] is preferably 7.89 mol%, more preferably 9.85 mol%, even more preferably 11.8 mol%, and particularly preferably 12.75 mol%, from the viewpoint of excellent rubber elasticity at low temperatures. The upper limit of the content of structural units derived from α-olefin [A2] is preferably 21.89 mol%, more preferably 19.85 mol%, even more preferably 17.8 mol%, and particularly preferably 16.75 mol%, from the viewpoint of excellent crosslinking properties, sheet blocking resistance, and pellet handling properties. In other words, from the viewpoint of excellent sheet blocking resistance and pellet handling properties, flexibility, and rubber elasticity at low temperatures, the content of structural units derived from α-olefin [A2] is preferably 7.89 to 21.89 mol%, more preferably 9.85 to 19.85 mol%, even more preferably 11.8 to 17.8 mol%, and particularly preferably 12.75 to 16.75 mol%. The content ratio of structural units derived from α-olefin [A2] is, １ It can be measured using H-NMR. Specifically, it can be determined by the method described in the examples below.

[0045] <Requirement (a3)> The copolymer (A) of the present invention has a content of structural units derived from non-conjugated polyene [A3] of 0.1 to 1.0 mol%, where 100 mol% is the sum of the structural units of [A1], [A2], and [A3], i.e., the sum of structural units derived from ethylene [A1], structural units derived from α-olefin [A2], and structural units derived from non-conjugated polyene [A3].

[0046] The lower limit of the content of structural units derived from non-conjugated polyene [A3] is preferably 0.11 mol%, more preferably 0.15 mol%, even more preferably 0.20 mol%, and particularly preferably 0.25 mol%, from the viewpoint of excellent crosslinking properties. The upper limit of the content of structural units derived from non-conjugated polyene [A3] is preferably 0.9 mol%, more preferably 0.8 mol%, even more preferably 0.7 mol%, and particularly preferably 0.6 mol%, from the viewpoint of excellent sheet blocking resistance and pellet handling properties. That is, the content of structural units derived from non-conjugated polyene [A3] is preferably 0.11 to 0.9 mol%, more preferably 0.15 to 0.8 mol%, even more preferably 0.20 to 0.7 mol%, and particularly preferably 0.25 to 0.6 mol%, from the viewpoint of excellent crosslinking properties, sheet blocking resistance of the sealing sheet, and pellet handling properties. The content of structural units derived from non-conjugated polyene [A3] is １ It can be measured using H-NMR. Specifically, it can be determined by the method described in the examples below.

[0047] The molar ratio [[A1] / [A2]] of structural units derived from ethylene [A1] to structural units derived from α-olefin [A2] in the copolymer (A) of the present invention is preferably 75.0 / 25.0 to 95.0 / 5.0, more preferably 78.1 / 21.9 to 92.1 / 7.9, even more preferably 80.1 / 19.9, particularly preferably 82.2 / 17.8, and most preferably 83.2 / 16.8, from the viewpoint of excellent rubber elasticity and sheet blocking resistance at low temperatures. The lower limit of the molar ratio [[A1] / [A2]] is preferably 75.0 / 25.0, more preferably 78.1 / 21.9, even more preferably 80.1 / 19.9, particularly preferably 82.2 / 17.8, and most preferably 83.2 / 16.8, from the viewpoint of excellent sheet blocking resistance. The upper limit of the molar ratio [[A1] / [A2]] is more preferably 92.1 / 7.9, even more preferably 90.1 / 9.9, particularly preferably 88.2 / 11.8, and most preferably 87.2 / 12.8, from the viewpoint of excellent rubber elasticity at low temperatures.

[0048] The molar ratio [[A1] / [A3]] of structural units derived from ethylene [A1] and structural units derived from non-conjugated polyene [A3] in the copolymer (A) of the present invention is preferably 100 to 1200, more preferably 120 to 1100, even more preferably 140 to 1000, particularly preferably 160 to 900, and most preferably 180 to 800, from the viewpoint of excellent crosslinkability and sheet blocking resistance. The molar ratios [[A1] / [A2]] and [[A1] / [A3]] are, １ It can be measured using H-NMR.

[0049] The copolymer (A) of the present invention preferably satisfies one or more of the following requirements (a4) to (a6) in addition to the above requirements (a1) to (a3), more preferably satisfies two or more of the following requirements (a4) to (a6), and even more preferably satisfies all of the following requirements (a4) to (a6). (a4) The melt flow rate measured at 190°C and a 2.16 kg load in accordance with ASTM D1238 is 3 to 20 g / 10 min. (a5) MFR １０ / MFR ２ However, it is in the range of 5.0 to 8.0 (MFR １０ This is the melt flow rate measured at 190°C and a 10 kg load in accordance with ASTM D1238, and MFR ２ This is the melt flow rate measured at 190°C and a 2.16 kg load in accordance with ASTM D1238. (a6) The glass transition temperature (Tg) measured by differential scanning calorimetry (DSC) is -50°C or lower.

[0050] <Requirement (a4)> The melt flow rate (MFR) of copolymer (A) of the present invention, measured at 190°C and a 2.16 kg load in accordance with ASTM D1238. ２ The amount is preferably 3 to 20 g / 10 min. Melt flow rate (MFR) ２ The lower limit of the melt flow rate (MFR) is more preferably 4.0 g / 10 min, even more preferably 5.0 g / 10 min, particularly preferably 6.0 g / 10 min, especially preferably 7.0 g / 10 min, and most preferably 8.0 g / 10 min. ２The upper limit of ) is more preferably 18 g / 10 min, even more preferably 16 g / 10 min, and particularly preferably 14 g / 10 min. That is, the melt flow rate (MFR ２ The melt flow rate (MFR) of copolymer (A) of the present invention is more preferably 4.0 to 20 g / 10 min, even more preferably 5.0 to 20 g / 10 min, particularly preferably 6.0 to 18 g / 10 min, especially preferably 7.0 to 16 g / 10 min, and most preferably 8.0 to 14 g / 10 min. ２ The melt flow rate (MFR) tends to decrease as the molecular weight increases. ２ If the above upper limit is below, then molded articles and crosslinked foams with superior strength can be easily obtained, and MFR ２ If the value is above the lower limit, the fluidity of the copolymer (A) during melt molding is improved.

[0051] <Requirement (a5)> MFR of copolymer (A) of the present invention １０ / MFR ２ The value is preferably 5.0 to 8.0. Here, MFR １０ This is the melt flow rate (g / 10 min) measured at 190°C and a 10 kg load in accordance with ASTM D1238, and MFR ２ This is the melt flow rate (g / 10 min) measured at 190°C and a load of 2.16 kg, in accordance with ASTM D1238. １０ / MFR ２ The lower limit is preferably 5.2, more preferably 5.5, even more preferably 5.7, and particularly preferably 6.0. Also, MFR １０ / MFR ２ The upper limit is preferably 7.9, more preferably 7.8. That is, MFR １０ / MFR ２ Preferably, it is 5.2 to 7.9, more preferably 5.5 to 7.9, even more preferably 5.7 to 7.8, and particularly preferably 6.0 to 7.8.

[0052] MFR １０ / MFR ２ This value is considered to be one of the indicators of the degree of long-chain branching in copolymers, and MFR １０ / MFR２ If the value falls within the aforementioned range, it can be said that it has long-chain branching. MFR １０ / MFR ２ A smaller value indicates fewer long-chain branches. (MFR) １０ / MFR ２ When a resin composition containing copolymer (A) whose value is equal to or greater than the aforementioned lower limit is crosslinked to produce a crosslinked body, the resulting crosslinked body tends to have high shape accuracy and excellent dimensional stability. １０ / MFR ２ When using copolymer (A) whose value is below the aforementioned upper limit, the resulting crosslinked material tends to have superior mechanical strength.

[0053] <Requirement (a6)> The glass transition temperature (Tg) of the copolymer (A) of the present invention, as measured by differential scanning calorimetry (DSC), is preferably -50°C or lower, from the viewpoint of excellent rubber elasticity at low temperatures. The upper limit of the glass transition temperature (Tg) is more preferably -55°C or lower, even more preferably -57°C or lower, and particularly preferably -60°C or lower. The lower limit of the glass transition temperature (Tg) is not particularly limited, but is usually -90°C or higher. The glass transition temperature (Tg) can be determined by the method described in the examples below.

[0054] <Method for Producing Copolymer (A)> The copolymer (A) of the present invention can be synthesized by various known production methods, for example, by conventionally known production methods using a metallocene catalyst. Examples of metallocene catalysts and production methods using the catalyst can be found in, for example, International Publication No. 2015 / 122415, particularly in paragraphs

[0249] to

[0320] of the said publication. Specifically, as described in the examples below, it can be obtained by copolymerizing at least ethylene [A], an α-olefin having 4 or more carbon atoms [B], and a non-conjugated polyene [C] in the presence of a metallocene catalyst.

[0055] The copolymer (A) of the present invention may contain structural units derived from at least one biomass-derived monomer. That is, the biomass-derived monomer used as a raw material for copolymer (A) may be biomass-derived ethylene, biomass-derived α-olefin having 4 or more carbon atoms, or biomass-derived non-conjugated polyene. The monomer used as a raw material for copolymer (A) of the present invention may contain both biomass-derived monomers and fossil fuel-derived monomers. It is preferable from the viewpoint of reducing environmental impact that the copolymer (A) of the present invention contains structural units derived from biomass-derived monomers.

[0056] Here, "biomass-derived" means that it can be obtained from any renewable natural raw materials and their residues, including fungi, yeasts, algae, and bacteria, whether plant-derived or animal-derived. Biomass-derived monomers such as ethylene, α-olefins with 4 or more carbon atoms, and unconjugated polyenes can be obtained by known methods. Biomass-derived monomers are carbon １４ 1 × 10¹¹ C isotopes －１２ ~1 x 10 －１４ While it contains a certain proportion, the corresponding monomers derived from fossil fuels are １４ Due to the radioactive decay of C １４ It is known that C is not included. Therefore, monomers derived from biomass and monomers derived from fossil fuels are different. １４ They can be distinguished by whether or not they contain a carbon isotope. Furthermore, copolymer (A) of the present invention may contain structural units derived from at least one type of chemically recycled monomer. That is, the chemically recycled monomer that serves as the raw material for copolymer (A) may be chemically recycled ethylene, chemically recycled α-olefin having 4 or more carbon atoms, or chemically recycled non-conjugated polyene.

[0057] The monomers used as raw materials for copolymer (A) of the present invention may consist solely of monomers derived from chemical recycling, or they may consist of both monomers derived from chemical recycling and monomers derived from fossil fuels. It is preferable for copolymer (A) of the present invention to contain structural units derived from monomers derived from chemical recycling from the viewpoint of reducing environmental impact (mainly waste reduction). Here, "derived from chemical recycling" means obtained by depolymerizing, thermally decomposing, etc., polymers such as waste plastics, or obtained by first converting polymers such as waste plastics into intermediates by depolymerizing, thermally decomposing, etc., and then producing the copolymer using these intermediates as raw materials. Monomers derived from chemical recycling, such as ethylene, α-olefins with 4 or more carbon atoms, and non-conjugated polyenes, can be obtained by known methods.

[0058] The form of the copolymer (A) of the present invention is not particularly limited as long as it does not impair the effects of the present invention, but examples include pellets and sheets.

[0059] 《Pellets》 The pellets of the present invention (hereinafter also referred to as "the pellets") contain the copolymer (A) of the present invention. The pellets are obtained, for example, by kneading and granulating the copolymer (A) of the present invention using an extruder equipped with a pelletizer. The pellets have excellent blocking resistance, thus suppressing pellet handling difficulties and maintaining a good pellet shape. In other words, the pellets have excellent pellet handling properties. The pellets may contain components other than copolymer (A) to the extent that they do not impair the effects of the present invention. Examples of components other than copolymer (A) include the components described later.

[0060] 《Resin Composition》 In the first embodiment of the resin composition of the present invention (hereinafter also referred to as "this composition"), it comprises a copolymer (A), an organic peroxide (B), and a silane coupling agent (C). In the second embodiment, it comprises a copolymer (A), a hydrosilyl group-containing compound (D), and a platinum-based catalyst (E).

[0061] <First Embodiment> The first embodiment of the composition comprises a copolymer (A), an organic peroxide (B), and a silane coupling agent (C). The copolymer (A), organic peroxide (B), and silane coupling agent (C) may each be present individually or in combination of two or more types.

[0062] The first embodiment of this composition preferably comprises 100 parts by mass of copolymer (A), 0.2 to 2.0 parts by mass of organic peroxide (B), and 0.10 to 4.0 parts by mass of silane coupling agent (C), from the viewpoint of excellent crosslinking performance at high temperatures (e.g., 70°C or higher) and from the viewpoint of performing the crosslinking reaction accurately, more preferably comprises 100 parts by mass of copolymer (A), 0.3 to 1.5 parts by mass of organic peroxide (B), and 0.12 to 2.0 parts by mass of silane coupling agent (C), and even more preferably comprises 100 parts by mass of copolymer (A), 0.4 to 1.0 parts by mass of organic peroxide (B), and 0.15 to 0.5 parts by mass of silane coupling agent (C).

[0063] [Organic Peroxide (B)] The first embodiment of this composition includes an organic peroxide (B). The organic peroxide (B) acts as a radical initiator to graft-modify the copolymer (A) of the present invention with a silane coupling agent (C). The graft-modified copolymer (A) is suitable as a encapsulant because it readily adheres to glass, backsheets, elements, electrodes, etc. The organic peroxide (B) also acts as a radical initiator to crosslink copolymers (A) together. The crosslinked copolymer (A) is suitable as a encapsulant because it has excellent heat resistance.

[0064] The 1-minute half-life temperature of the organic peroxide (B) is preferably 100 to 170°C, more preferably 120 to 165°C, from the viewpoint of balancing productivity during calendering and crosslinking rate during lamination.

[0065] Organic peroxides with a one-minute half-life temperature of 100°C or higher can suppress the generation of gel when producing uncrosslinked sheets from this composition using a calendering machine. This suppresses deterioration of appearance due to the generation of irregularities on the sheet surface. Furthermore, when the crosslinked body is used as a encapsulant, it can suppress the decrease in dielectric breakdown resistance due to crack generation around the gel when voltage is applied, and also suppress the decrease in moisture permeability at the gel interface. In addition, it can suppress the decrease in adhesion to glass, solar cell elements, electrodes, and backsheets due to the generation of irregularities on the surface of the encapsulant. Moreover, when this composition is stored for a long period of time, it can suppress the decrease in fluidity during lamination due to the progress of the crosslinking reaction within the composition. Organic peroxide (B) with a one-minute half-life temperature of 170°C or lower can suppress the decrease in the crosslinking rate of this resin composition when obtaining a crosslinked body, thereby increasing the productivity of the crosslinked body.

[0066] Organic peroxides (B) include dilauroyl peroxide, 1,1,3,3-tetramethylbutylperoxy-2-ethylhexanoate, dibenzoyl peroxide, tert-amylperoxy-2-ethylhexanoate, tert-butylperoxy-2-ethylhexanoate, tert-butylperoxyisobutyrate, tert-butylperoxymaleic acid, 1,1-di(tert-amylperoxy)-3,3,5-trimethylcyclohexane, 1,1-di(tert-amylperoxy)cyclohexane, tert-amylperoxyisononanoate, tert-amylperoxyn-octoate, 1,1-di(tert-butylperoxy)-3,3,5-trimethylcyclohexane, and 1,1-di(tert-butylperoxy Examples include cyclohexane, tert-butyl peroxyisopropyl carbonate, tert-butyl peroxy-2-ethylhexyl carbonate, 2,5-dimethyl-2,5-di(benzoylperoxy)hexane, tert-amyl-peroxybenzoate, tert-butyl peroxyacetate, tert-butyl peroxyisononanoate, 2,2-di(tert-butylperoxy)butane, tert-butyl peroxybenzoate, etc., and dilauroyl peroxide, tert-butyl peroxyisopropyl carbonate, tert-butyl peroxyacetate, tert-butyl peroxyisononanoate, tert-butyl peroxy-2-ethylhexyl carbonate, and tert-butyl peroxybenzoate. Among these, tert-butyl peroxy-2-ethylhexyl carbonate is preferred.

[0067] If the content of organic peroxide (B) in the first embodiment of this composition is 0.2 parts by mass or more, the crosslinkability of the composition is improved. Furthermore, the graft reaction of the silane coupling agent (C) to the copolymer (A) proceeds more readily, resulting in excellent heat resistance and adhesion to glass, backsheets, elements, electrodes, etc., of the resulting crosslinked material. If the content of organic peroxide (B) in the first embodiment of this composition is 2.0 parts by mass or less, the generation of gel material when producing an uncrosslinked sheet from this composition using a calendering machine can be suppressed.

[0068] [Silane Coupling Agent (C)] The first embodiment of this composition includes a silane coupling agent (C). The silane coupling agent (C) can be any conventionally known agent and is not particularly limited. Specific examples of the silane coupling agent (C) include vinyltriethoxysilane, vinyltrimethoxysilane, vinyltris(β-methoxyethoxysilane), γ-glycidoxypropyltrimethoxysilane, γ-aminopropyltriethoxysilane, γ-methacryloxypropyltrimethoxysilane, etc. From the viewpoint of improving the adhesion of the crosslinked body to the glass, backsheet, elements and electrodes, etc., γ-glycidoxypropylmethoxysilane, γ-aminopropyltriethoxysilane, γ-methacryloxypropyltrimethoxysilane, and vinyltriethoxysilane are preferred, and γ-methacryloxypropyltrimethoxysilane is more preferred.

[0069] If the silane coupling agent (C) in the first embodiment of this composition is 0.1 parts by mass or more, the adhesion of the resulting crosslinked body to glass, backsheets, elements, electrodes, etc., is improved. If the silane coupling agent (C) in the first embodiment of this composition is 4.0 parts by mass or less, the balance between cost and performance can be improved when the resulting crosslinked body is used as a encapsulant for solar cells.

[0070] <Second Embodiment> The second embodiment of this composition comprises a copolymer (A), a hydrosilyl group-containing compound (D), and a platinum-based catalyst (E). The copolymer (A), the hydrosilyl group-containing compound (D), and the platinum-based catalyst (E) may each be present individually or in combination of two or more. The second embodiment of this composition is suitable as a encapsulant for perovskite solar cells because it enables crosslinking reactions at low temperatures (e.g., 130°C or below) that can suppress the decomposition of heat-sensitive perovskite compounds.

[0071] The content of the hydrosilyl group-containing compound (D) in the second embodiment of this composition is preferably 0.1 to 100 parts by mass, more preferably 0.5 to 50 parts by mass, even more preferably 1.0 to 30 parts by mass, and particularly preferably 1.5 to 10 parts by mass, per 100 parts by mass of copolymer (A). The content of the platinum-based catalyst (E) in the second embodiment of this composition is preferably 0.000001 to 5 parts by mass, more preferably 0.00001 to 0.5 parts by mass, even more preferably 0.0001 to 0.05 parts by mass, and particularly preferably 0.001 to 0.007 parts by mass, per 100 parts by mass of copolymer (A).

[0072] In a second embodiment of this composition, the copolymer (A) is hydrosilicone crosslinked using a hydrosilyl group-containing compound (D). As a result, the resulting crosslinked material exhibits good light transmittance and volume resistivity, similar to crosslinking using peroxides, while also exhibiting good crosslinkability even at low temperatures (e.g., 130°C or below).

[0073] A second embodiment of the present composition may further contain a silane coupling agent (C). Specific examples and preferred forms of the silane coupling agent (C) are as described above. When the second embodiment of the present composition contains a silane coupling agent (C), the content of the silane coupling agent (C) per 100 parts by mass of copolymer (A) may be 0.10 to 4.0 parts by mass, 0.12 to 2.0 parts by mass, or 0.15 to 0.5 parts by mass.

[0074] [Hydrosilyl group-containing compound (D)] The second embodiment of this composition comprises a hydrosilyl group-containing compound (D). The hydrosilyl group-containing compound (D) is preferably an organohydrogenpolysiloxane represented by the following general formula (d) (hereinafter also referred to as "compound (d)"). Compound (d) has at least one silicon atom-bonded aralkyl group and at least two silicon atom-bonded hydrogen atoms in its molecule.

[0075]

[0076] The definitions of each sign in equation (d) are as follows: n and p are independently 0 or positive integers. m is an integer between 1 and 20. The sum of n, m, and p is between 5 and 50. Multiple R １ and R ２ Each of these is independently a monovalent alkyl group. There are multiple R １ These are independently monovalent alkyl groups. There are multiple R ２ R is independently a monovalent alkyl group. １ R ２ It may be the same alkyl group as above, or a different alkyl group. In the alkyl group, some of the hydrogen atoms bonded to carbon atoms may be substituted with halogen atoms. R a This is an aralkyl group. The two Rs are independently hydrogen atoms, R １ , R ２ , and R ａ Selected from the group consisting of the following. However, when n=1, at least one of the two R is a hydrogen atom, and when n=0, both of the two R are hydrogen atoms. R is preferably R １ or R ２ That is the case.

[0077] The hydrosilyl group-containing compound (D) is a linear organohydrogenpolysiloxane having a relatively low degree of siloxane polymerization and containing at least one silicon atom-bonded aralkyl group and at least two silicon atom-bonded hydrogen atoms within its molecule.

[0078] In compound (d), a diorganosiloxy unit having a silicon atom bonded aralkyl group (-[O-Si(R １ ) (Caution ａ ) ]-), organohydrogensiloxy unit having a silicon atom bonded to a hydrogen atom (-[O-Si(R １ )H]-), and silicon atom bonded aralkyl groups and diorganosiloxy units (-[O-Si(R) that do not contain silicon atom bonded hydrogen atoms １ ) (Caution ２Siloxy units such as ) and )]-) may be arranged in a block-like manner or randomly. In other words, the arrangement order of the siloxy units in compound (d) is not particularly limited.

[0079] In formula (d), m is the number of diorganosiloxy units having silicon atom bonded aralkyl groups, and is an integer from 1 to 20, preferably an integer from 2 to 10, and more preferably an integer from 3 to 6.

[0080] In formula (d), n is the number of organohydrogensiloxy units having silicon-bonded hydrogen atoms. n may be 0 or 1, but when n=1, at least one of the two R atoms is a hydrogen atom, and when n=0, both R atoms are hydrogen atoms. That is, compound (d) has a structure containing at least two silicon-bonded hydrogen atoms in one molecule. Note that even if n is a number other than 0 or 1, it is not prevented that one or both of the R atoms at both ends of the molecular chain are silicon-bonded hydrogen atoms. Preferably, n is an integer other than 0 or 1, and n ≥ m. More preferably, n is an integer from 3 to 10, and even more preferably from 3 to 9.

[0081] In formula (d), p is the number of diorganosiloxy units that do not contain silicon atom-bonded aralkyl groups or silicon atom-bonded hydrogen atoms. p may be 0, or it may be the number obtained by subtracting the values ​​of n and m from the total degree of polymerization of siloxy units, which is expressed as the sum of n, m, and p described later. p is preferably 0 or an integer from 1 to 12, more preferably 0 or an integer from 1 to 10, even more preferably 0 or an integer from 1 to 5, and particularly preferably 0 or an integer from 1 to 2.

[0082] The hydrosilyl group-containing compound (D) has a relatively low degree of siloxane polymerization, and the sum of the values ​​of n, m, and p is 5 to 50, preferably 5 to 20, and more preferably 5 to 15. In formula (d), a particularly preferred embodiment is that m is an integer from 3 to 6, n is an integer from 3 to 9, and p is an integer from 0 to 1 to 2.

[0083] In equation (d), R is a hydrogen atom, R １ , R ２, and R ａ It may be any group selected from the group consisting of the following. However, if n = 0 or 1, both or one of R is a hydrogen atom.

[0084] In equation (d), R １ and R ２ The group is a monovalent alkyl group, which may be the same or different, and some of the carbon atom-bonded hydrogen atoms may be substituted with halogen atoms. Preferably, such alkyl groups are C1 to C20 alkyl groups, more preferably C1 to C10 alkyl groups, and even more preferably C1 to C5 alkyl groups, with a methyl group being particularly preferred industrially.

[0085] In equation (d), R ａ The group is an aralkyl group, preferably an aralkyl group having 7 to 20 carbon atoms, more preferably an aralkyl group having 7 to 15 carbon atoms. Examples of such aralkyl groups include benzyl group, phenylethyl group, phenylpropyl group, and phenylbutyl group. Among these, the group between the aryl group such as the phenyl group and the silicon atom is -CH(CH ３ A preferred aralkyl group contains at least one branched unit represented by ). ａ A particularly preferred embodiment is -CH ２ -CH(CH ３ )-C ６ H ５ This is an aralkyl group represented by [formula].

[0086] The aralkyl group is a characteristic functional group that gives hydrosilyl group-containing compounds (D) usefulness as crosslinking agents. In particular, when aralkyl groups are present together with silicon-bonded hydrogen atoms in hydrosilyl group-containing compounds (D) where n, m, and p are within the above ranges, the physical properties of the resulting crosslinked material tend to be significantly improved. By using hydrosilyl group-containing compounds (D) in combination with copolymers (A), crosslinked materials with particularly excellent physical properties such as moldability, elongation at fracture, and compression molding strain can be obtained.

[0087] [Platinum-based catalyst (E)] The second embodiment of this composition includes a platinum-based catalyst (E). Platinum-based catalysts for hydrosilicone crosslinking are widely used in hydrosilicone crosslinking reactions involving the addition reaction of silicon-bonded hydrogen atoms to carbon-carbon double bonds using a hydrosilyl group-containing compound (D). The platinum-based catalyst for hydrosilicone crosslinking is an addition reaction catalyst, and the platinum-based catalyst (E) can be used without particular limitations as long as it promotes the addition reaction (hydrosilylation reaction of alkenes) between the carbon-carbon double bond (e.g., alkenyl group) of the copolymer (A) of the present invention and the hydrosilyl group of the hydrosilyl group-containing compound (D).

[0088] Examples of platinum-based catalysts (E) include finely powdered metal platinum catalysts described in U.S. Patent No. 2,970,150, etc., chloroplatinic acid catalysts described in U.S. Patent No. 2,823,218, etc., complex compounds of platinum and hydrocarbons described in U.S. Patent No. 3,159,601 and U.S. Patent No. 159,662, etc., complex compounds of chloroplatinic acid and olefins described in U.S. Patent No. 3,516,946, etc., and complex compounds of platinum and vinylsiloxanes described in U.S. Patent No. 3,775,452 and U.S. Patent No. 3,814,780, etc.

[0089] Examples of platinum-based catalysts (E) include elemental platinum (platinum black); platinum complexes such as chloroplatinic acid, platinum-hydrocarbon complexes, platinum-vinylsiloxane complexes, platinum-alcohol complexes, chloroplatinic acid-olefin complexes, and chloroplatinic acid-vinylsiloxane complexes. Among these, platinum-vinylsiloxane complexes are preferred due to their high catalytic activity. An example of a platinum-vinylsiloxane complex is 1,1,3,3-tetramethyl-1,3-divinyldisiloxane platinum complex. The platinum-based catalyst (E) may be supported on a carrier such as alumina or silica.

[0090] [Reaction Inhibitor (F)] The second embodiment of this composition may further contain a reaction inhibitor (F). The reaction inhibitor (F) is a compound that has the function of suppressing the crosslinking reaction (hydrosilylation reaction of alkenes) between the carbon-carbon double bond (e.g., alkenyl group) contained in copolymer (A) and the hydrosilyl group contained in hydrosilyl group-containing compound (D). This composition containing the reaction inhibitor (F) tends to stabilize the processability during kneading and molding.

[0091] Examples of reaction inhibitors (F) include benzotriazole; acetylene alcohols such as 1-hexyn-3-ol, 3-methyl-1-butyn-3-ol, 3,6-dimethyl-4-octin-3,6-diol, 2,4,7,9-tetramethyl-5-decine-4,7-diol, 1-ethynyl-1-cyclohexanol, and 3,5-dimethyl-1-hexyn-3-ol; acrylonitrile; and N,N-diallyl acetylene alcohols. Amide compounds such as toamide, N,N-diallylbenzamide, N,N,N',N'-tetraallyl-o-phthalate diamide, N,N,N',N'-tetraallyl-m-phthalate diamide, and N,N,N',N'-tetraallyl-p-phthalate diamide; and other examples include sulfur, phosphorus, nitrogen, amine compounds, sulfur compounds, phosphorus compounds, tin, tin compounds, and tetramethyltetravinylcyclotetrasiloxane. Among these, 1-ethynyl-1-cyclohexanol is preferred.

[0092] If the composition contains a reaction inhibitor (F), the amount of reaction inhibitor (F) in the composition is preferably 0.001 to 5 parts by mass, more preferably 0.005 to 4 parts by mass, and even more preferably 0.05 to 3 parts by mass, per 100 parts by mass of copolymer (A).

[0093] [Adhesion-imparting agent (G)] The second embodiment of this composition may further include an adhesion-imparting agent (G). The adhesion-imparting agent (G) is a silane-modified resin, and is preferably a silane-modified resin obtained by graft polymerization of a polymerizable silane compound such as an ethylenically unsaturated silane compound onto a resin which is the main component.

[0094] The main constituent resins include ethylene homopolymers and copolymers of ethylene and at least one copolymer component other than ethylene (hereinafter also referred to as "ethylene copolymers"). The ethylene copolymer may be a random copolymer of ethylene and a copolymer component, or a block copolymer, but a random copolymer is preferred. Examples of copolymer components in ethylene copolymers include α-olefins, cyclic olefins, vinyl acetate, etc., with 3 to 20 carbon atoms.

[0095] Examples of α-olefins with 3 to 20 carbon atoms include propylene, 1-butene, 1-pentene, 1-hexene, 4-methyl-1-pentene, 1-octene, 1-decene, 1-dodecene, 1-tetradecene, 1-hexadecene, 1-octadecene, and 1-eicosene.

[0096] Examples of cyclic olefins include norbornene derivatives, tricyclo-3-decene derivatives, tricyclo-3-undecene derivatives, tetracyclo-3-dodecene derivatives, pentacyclo-4-pentadecene derivatives, pentacyclopentadecadiene derivatives, pentacyclo-3-pentadecene derivatives, pentacyclo-4-hexadecene derivatives, pentacyclo-3-hexadecene derivatives, hexacyclo-4-heptadecene derivatives, heptacyclo-5-eicosene derivatives, and heptasi This includes chloro-4-eicosene derivatives, heptacyclo-5-heneicosene derivatives, octacyclo-5-docosene derivatives, nonacyclo-5-pentacosene derivatives, nonacyclo-6-hexacosene derivatives, cyclopentadiene-acenaphthylene adducts, 1,4-methano-1,4,4a,9a-tetrahydrofluorene derivatives, 1,4-methano-1,4,4a,5,10,10a-hexahydroanthracene derivatives, and cycloalkylene derivatives having 3 to 20 carbon atoms. Among these, tetracyclo[4.4.0.12,5.17,10]-3-dodecene derivatives and hexacyclo[6.6.1.13,6.110,13.02,7.09,14]-4-heptadecene derivatives are preferred, with tetracyclo[4.4.0.12,5.17,10]-3-dodecene being more preferred.

[0097] The copolymer components (α-olefin, cyclic olefin, and vinyl acetate) in the ethylene copolymer may be used individually or in combination of two or more. From the viewpoint of adhesion, silane-modified resins having reactive groups such as alkoxy groups or halogen groups bonded to silicon atoms are preferably used. The higher the activity of the reactive groups in the silane-modified resin and the greater the number of reactive groups, the better the adhesion.

[0098] The method for producing the silane-modified resin is not particularly limited, but it is preferable to produce it by graft polymerization of the main component resin and a polymerizable silane compound using an organic peroxide. By graft polymerization with the main component resin as the main chain and the polymerizable silane compound as the side chain, the degree of freedom of reactive groups such as alkoxyl groups in the polymerizable silane compound that contribute to adhesive strength is increased, and the adhesion to the surface of surface protective members and the like in the solar cell module is improved more efficiently.

[0099] The polymerizable silane compounds mentioned above can be conventionally known compounds and are not particularly limited, but ethylenically unsaturated silane compounds can be used. Specific examples of ethylenically unsaturated silane compounds include vinyltriethoxysilane, vinyltrimethoxysilane, vinyltris(β-methoxyethoxysilane), γ-glycidoxypropyltrimethoxysilane, γ-aminopropyltriethoxysilane, and γ-methacryloxypropyltrimethoxysilane.

[0100] The amount of modification by the polymerizable silane compound described above is typically 0.1 to 5 parts by mass, preferably 0.1 to 4 parts by mass, per 100 parts by mass of the main component resin, from the viewpoint of achieving an excellent balance between adhesion and flexibility.

[0101] If the composition contains an adhesion promoter (G), the content of the adhesion promoter (G) in the composition is preferably 5 to 50 parts by mass, more preferably 10 to 40 parts by mass, even more preferably 15 to 35 parts by mass, and even more preferably 20 to 30 parts by mass, per 100 parts by mass of copolymer (A).

[0102] <Other Components> In both the first and second embodiments described above, this composition may contain other components as long as they do not impair the effects of the present invention, depending on the desired purpose. For example, it may contain additives selected from polyolefins other than the copolymer (A) of the present invention, various resins and / or various rubbers other than polyolefins, organic peroxides (B) and hydrosilyl group-containing compounds (D), crosslinking agents other than weather stabilizers, crosslinking aids, vulcanization accelerators, vulcanization aids, reinforcing agents, plasticizers, tackifiers, fillers, softeners, anti-aging agents, processing aids, activators, hygroscopic agents, foaming agents, heat stabilizers, antistatic agents, antibacterial agents, antifungal agents, flame retardants, dispersants, colorants, pigments, dyes, lubricants, and thickeners. Each additive may be present individually or in combination of two or more.

[0103] (Polyolefins other than copolymer (A)) Examples of polyolefins other than copolymer (A) of the present invention include styrene-based and ethylene-based block copolymers, propylene-based polymers, and the like. When using polymers other than copolymer (A) of the present invention, the amount of polymer other than copolymer (A) of the present invention is usually 0.0001 to 50 parts by mass per 100 parts by mass of copolymer (A), and may be 0.001 to 40 parts by mass.

[0104] (Crosslinking agents other than organic peroxide (B) and hydrosilyl group-containing compound (D)) In addition to the crosslinking agent (organic peroxide (B)) disclosed in the first embodiment and the crosslinking agent (hydrosilyl group-containing compound (D)) disclosed in the second embodiment, this composition may also use crosslinking agents that are commonly used when crosslinking rubber. Examples of such crosslinking agents include phenolic resins, sulfur compounds, amino resins, quinones or their derivatives, amine compounds, azo compounds, epoxy compounds, isocyanate compounds, etc. The first and second embodiments may be combined.

[0105] (Weathering stabilizer) For example, conventionally known compounds can be used as a weathering stabilizer, such as a light stabilizer, antioxidant, or ultraviolet absorber. When a weathering stabilizer is used, the amount of the weathering stabilizer is preferably 0.01 to 2.0 parts by mass, more preferably 0.05 to 1.0 parts by mass, and even more preferably 0.07 to 0.5 parts by mass, per 100 parts by mass of copolymer (A). When the amount of the weathering stabilizer is within the above range, it tends to sufficiently ensure the effect of improving resistance to constant temperature and humidity, resistance to high temperature and humidity, resistance to heat cycles, weathering stability, and heat resistance, and also prevents a decrease in adhesion between the crosslinked body and the glass, backsheet, elements, electrodes, etc.

[0106] Examples of light stabilizers include 2,2,6,6-tetramethyl-4-piperidyl stearate, 1,2,2,6,6-pentamethyl-4-piperidyl stearate, 2,2,6,6-tetramethyl-4-piperidyl benzoate, N-(2,2,6,6-tetramethyl-4-piperidyl)dodecyl succinimide, 1-[(3,5-di-tert-butyl-4-hydroxyphenyl)propionyloxyethyl]-2,2,6,6-tetramethyl-4-piperidyl-(3,5-di-tert-butyl-4-hydroxyphenyl)propionate, bis(1,2,2,6,6 -Pentamethyl-4-piperidyl) sebacate, bis(1,2,2,6,6-pentamethyl-4-piperidyl)-2-butyl-2-(3,5-diter-butyl-4-hydroxybenzyl) malonate, N,N'-bis(2,2,6,6-tetramethyl-4-piperidyl) hexamethylenediamine, tetrakis(2,2,6,6-tetramethyl-4-piperidyl)-1,2,3,4-butanetetracarboxylate, tetrakis(1,2,2,6,6-pentamethyl-4-piperidyl)-1,2,3,4-butanetetracarboxylate, bis(2,2, 6,6-tetramethyl-4-piperidyl) di(tridecyl)-1,2,3,4-butanetetracarboxylate, bis(1,2,2,6,6-pentamethyl-4-piperidyl) di(tridecyl)-1,2,3,4-butanetetracarboxylate, 3,9-bis[1,1-dimethyl-2-{tris(2,2,6,6-tetramethyl-4-piperidyloxycarbonyloxy)butylcarbonyloxy}ethyl]-2,4,8,10-tetraoxaspiro[5.5]undecane, 3,9-bis[1,1-dimethyl-2-{tris(1,2,2,6,6 -Pentamethyl-4-piperidyloxycarbonyloxy)butylcarbonyloxy}ethyl]-2,4,8,10-tetraoxaspiro[5.5]undecane, 1,5,8,12-tetrakis[4,6-bis{N-(2,2,6,6-tetramethyl-4-piperidyl)butylamino}-1,3,5-triazin-2-yl]-1,5,8,12-tetraazadodecane, 1-(2-hydroxyethyl)-2,2,6,6-tetramethyl-4-piperidinol / dimethyl succinate condensate, 2-tertiary octylamino-4,6-dichloro-s-triazine / N,N'-bis(2,2,6,6-tetramethyl-4-piperidyl)hexamethylenediamine condensate, N,N'-bis(2,2,6,6-tetramethyl-4-piperidyl)hexamethylenediamine / dibromoethane condensate, 2,2,6,6-tetramethyl-4-hydroxypiperidine-N-oxyl, bis(2,2,6,6-tetramethyl-N-oxylpiperidine)sebacate, tetrakis(2,2,6,6-tetramethyl-N-oxypiperidyl)butane-1,2,3,4-tetracarboxylate, 3,9-bis(1,1-dimethyl-2-(tris (2,2,6,6-tetramethyl-N-oxylpiperidyl-4-oxycarbonyl)butylcarbonyloxy)ethyl)2,4,6,10-tetraoxalospiro[5.5]undecane, 1,6-bis(2,2,6,6-tetramethyl-4-piperidylamino)hexane / dibromoethane polycondensate, 1,6-bis(2,2,6,6-tetramethyl-4-piperidylamino)hexane / 2,4-dichloro-6-tertiaryoctylamino-s-triazine polycondensate, 1,6-bis(2,2,6,6-tetramethyl-4-piperidylamino)hexane / 2,4- Dichloro-6-morpholino-s-triazine polycondensate, condensate of 2,2,6,6-tetramethyl-4-piperidinol, tridecyl alcohol, and 1,2,3,4-butanetetracarboxylic acid, condensate of 2,2,6,6-tetramethyl-4-piperidinol, condensate of 1,2,2,6,6-pentamethyl-4-piperidinol, tridecyl alcohol, and 1,2,3,4-butanetetracarboxylic acid, condensate of 1,2,2,6,6-pentamethyl-4-piperidinol, and 1,2,3,4-butanetetracarboxylic acid Compound, 1-[2-[3-(3,5-di-tert-butyl-4-hydroxyphenyl)propionyloxy]ethyl]-4-[3-3,5-di-tert-butyl-4-hydroxyphenyl]propionyloxy]-2,2,6,6-tetramethylpiperidine (e.g., Sanol LS-2626 (manufactured by Sankyo Co., Ltd.)), 2-(3,5-di-tert-butyl-4-hydroxybenzyl)-2-n-butylmalonic acid-bis-(1,2,2,6,6-pentamethyl-4-piperidyl) (e.g., Tinuvin 144 (manufactured by BASF)), bis(2,2,6,Examples include 6-tetramethyl-4-piperidyl)sebacate (e.g., TINUVIN 770 (BASF)) and poly[6-(1,1,3,3-tetramethylbutyl)imino-1,3,5-triazine-2,4-diyl][(2,2,6,6-tetramethyl-4-piperidyl)imino]hexamethylene[(2,2,6,6-tetramethyl-4-piperidyl)imino] (e.g., CHIMASSORB 944 (BASF)).

[0107] Examples of antioxidants include phenolic antioxidants, phosphorus-based antioxidants, sulfur-based antioxidants, and thioether-based antioxidants.

[0108] Examples of phenolic antioxidants include acrylate-based phenolic compounds described in Japanese Patent Publication No. 63-179953 and Japanese Patent Publication No. 1-168643, such as 2-tert-butyl-6-(3-tert-butyl-2-hydroxy-5-methylbenzyl)-4-methylphenyl acrylate and 2,4-di-tert-amyl-6-(1-(3,5-di-tert-amyl-2-hydroxyphenyl)ethyl)phenyl acrylate; 2,6-di-te rt-butyl-4-methylphenol, 2,6-di-tert-butyl-4-ethylphenol, octadecyl-3-(3,5-di-tert-butyl-4-hydroxyphenyl)propionate, 2,2'-methylene-bis(4-methyl-6-tert-butylphenol), 4,4'-butylidene-bis(6-tert-butyl-m-cresol), 4,4'-thiobis(3-methyl-6-tert-butylphenol), bis(3-cyclohexyl- 2-hydroxy-5-methylphenyl)methane, 3,9-bis(2-(3-(3-tert-butyl-4-hydroxy-5-methylphenyl)propionyloxy)-1,1-dimethylethyl)-2,4,8,10-tetraoxaspiro[5.5]undecane, 1,1,3-tris(2-methyl-4-hydroxy-5-tert-butylphenyl)butane, 1,3,5-trimethyl-2,4,6-tris(3,5-di-tert-butyl-4-hydroxymethylphenyl) Alkyl-substituted phenolic compounds such as benzene, tetrakis(methylene-3-(3',5'-di-tert-butyl-4'-hydroxyphenylpropionate)methane [i.e., pentaerythrimethyl-tetrakis(3-(3,5-di-tert-butyl-4-hydroxyphenylpropionate)], triethylene glycol bis(3-(3-tert-butyl-4-hydroxy-5-methylphenyl)propionate), and tocopherol;Examples of triazine group-containing phenolic compounds include 6-(4-hydroxy-3,5-di-tert-butylanilino)-2,4-bisoctylthio-1,3,5-triazine, 6-(4-hydroxy-3,5-dimethylanilino)-2,4-bisoctylthio-1,3,5-triazine, 6-(4-hydroxy-3-methyl-5-tert-butylanilino)-2,4-bisoctylthio-1,3,5-triazine, and 2-octylthio-4,6-bis-(3,5-di-tert-butyl-4-oxyanilino)-1,3,5-triazine. Among these, acrylate-based phenolic compounds and alkyl-substituted phenolic compounds are preferred, and alkyl-substituted phenolic compounds are more preferred.

[0109] Examples of phosphorus-based antioxidants include triphenyl phosphite, diphenylisodecyl phosphite, phenyl diisodecyl phosphite, tris(nonylphenyl) phosphite, tris(dinonylphenyl) phosphite, tris(2,4-di-tert-butylphenyl) phosphite, tris(2-tert-butyl-4-methylphenyl) phosphite, tris(cyclohexylphenyl) phosphite, and 2,2-methylenebis(4,6-di-tert-butylphenyl) Monophosphite compounds such as 10-(3,5-di-tert-butyl-4-hydroxybenzyl)-9,10-dihydro-9-oxa-10-phosphaphenanthrene-10-oxide, 10-decyloxy-9,10-dihydro-9-oxa-10-phosphaphenanthrene, and 4,4'-butylidene-bis(3-methyl-6-tert-butyl) Phenyl-di-tridecyl phosphite), 4,4'-isopropylidene-bis(phenyl-di-alkyl(C12-C15) phosphite), 4,4'-isopropylidene-bis(diphenyl monoalkyl(C12-C15) phosphite), 1,1,3-tris(2-methyl-4-di-tridecyl phosphite-5-tert-butylphenyl)butane, tetrakis(2,4-di-tert-butylphenyl)-4,4'-biphenylenediphosphite, cyclic Examples of diphosphite compounds include neopentanetetraylbis(isodecyl phosphite), cyclic neopentanetetraylbis(nonylphenyl phosphite), cyclic neopentanetetraylbis(2,4-di-tert-butylphenyl phosphite), cyclic neopentanetetraylbis(2,4-dimethylphenyl phosphite), and cyclic neopentanetetraylbis(2,6-di-tert-butylphenyl phosphite). Among these, monophosphite compounds are preferred, with tris(nonylphenyl) phosphite, tris(dinonylphenyl) phosphite, and tris(2,4-di-tert-butylphenyl) phosphite being more preferred.

[0110] Examples of sulfur-based antioxidants include dilauryl-3,3-thiodipropionate, dimyristyl-3,3'-thiodipropionate, distearyl-3,3-thiodipropionate, laurylstearyl-3,3-thiodipropionate, pentaerythritol-tetrakis-(β-lauryl-thio-propionate), and 3,9-bis(2-dodecylthioethyl)-2,4,8,10-tetraoxaspiro[5.5]undecane.

[0111] Examples of thioether-based antioxidants include tetrakis{methylene-3-(laurylthio)propionate}methane, bis[methyl-4-{3-n-alkyl(C12 or C14)thiopropioniodyl}-5-tert-butylphenyl]sulfide, and ditridecyl-3,3'-thiodipropionate.

[0112] Examples of UV absorbers include benzophenone-based UV absorbers, salicylic acid-based UV absorbers, benzotriazole-based UV absorbers, acrylate-based UV absorbers, and metal complex salt-based UV absorbers.

[0113] Examples of benzophenone-based UV absorbers include 2,4-dihydroxybenzophenone, 2-hydroxy-4-methoxybenzophenone, 2-hydroxy-4-methoxybenzophenone-5-sulfonic acid trihydrate, 2-hydroxy-4-octyloxybenzophenone, 4-dodecaloxy-2-hydroxybenzophenone, 4-benzyloxy-2-hydroxybenzophenone, 2,2',4,4'-tetrahydroxybenzophenone, and 2,2'-dihydroxy-4,4'-dimethoxybenzophenone.

[0114] Examples of salicylic acid-based UV absorbers include phenyl salchylate, 4-tert-butylphenyl-2-hydroxybenzoate, phenyl-2-hydroxybenzoate, 2,4-di-tert-butylphenyl-3,5-di-tert-butyl-4-hydroxybenzoate, and hexadecyl-3,5-di-tert-butyl-4-hydroxybenzoate.

[0115] Examples of benzotriazole-based UV absorbers include 2-(2-hydroxy-5-methylphenyl)2H-benzotriazole, 2-(3-tert-butyl-2-hydroxy-5-methylphenyl)-5-chloro-2H-benzotriazole, 2-(3,5-di-tert-butyl-2-hydroxyphenyl)-5-chloro-2H-benzotriazole, 2-(3,5-di-tert-butyl-2-hydroxyphenyl)-2H-benzotriazole, and 5-chloro-2-(3,5-di-tert-butyl-2-hydroxyphenyl)-2H-benzotriazole Examples include 2-(3,5-di-tert-amyl-2-hydroxyphenyl)-2H-benzotriazole, 2-(2-hydroxy-5-tert-octylphenyl)-2H-benzotriazole, 2-(2-hydroxy-4-octylphenyl)-2H-benzotriazole, 2-(2H-benzotriazole-2-yl)-4-methyl-6-(3,4,5,6-tetrahydrophthalimidylmethyl)phenol, and 2,2'-methylenebis[4-(1,1,3,3-tetramethylbutyl)-6-[(2H-benzotriazole-2-yl)phenol]].

[0116] Examples of acrylate-based ultraviolet absorbers include ethyl-2-cyano-3,3-diphenylacrylate and 2'-ethylhexyl-2-cyano-3,3-diphenylacrylate.

[0117] Commonly used as metal complex salt ultraviolet absorbers are complex salts of nickel and cobalt. Specifically, examples include nickel [2,2'-thiobis(4-tert-octyl)phenolate]n-butylamine, nickel dibutyldithiocarbamate, nickel bis[o-ethyl-3,5-(di-tert-butyl-4-hydroxybenzyl)]phosphate, cobalt dicyclohexyldithiophosphate, and [1-phenyl,3-methyl,4-decanonyl,pyrazolate(5)2]nickel.

[0118] (Crosslinking Aid) As the crosslinking aid, conventionally known crosslinking aids commonly used in olefin resins can be used. The crosslinking aid has a double bond in its molecule. The crosslinking aid suppresses the generation of air bubbles in the sealant after lamination and moderately enhances the crosslinkability.

[0119] Specifically, crosslinking aids include monoacrylates such as tert-butyl acrylate, lauryl acrylate, cetyl acrylate, stearyl acrylate, 2-methoxyethyl acrylate, ethyl carbitol acrylate, and methoxytripropylene glycol acrylate; monomethacrylates such as tert-butyl methacrylate, lauryl methacrylate, cetyl methacrylate, stearyl methacrylate, methoxyethylene glycol methacrylate, and methoxypolyethylene glycol methacrylate; diacrylates such as 1,4-butanediol diacrylate, 1,6-hexanediol diacrylate, 1,9-nonanediol diacrylate, neopentyl glycol diacrylate, diethylene glycol diacrylate, tetraethylene glycol diacrylate, polyethylene glycol diacrylate, tripylene glycol diacrylate, and polypropylene glycol diacrylate; and 1,3-butanediol dimethacrylate, 1,6-hexanediol dimethacrylate, and 1,9- Examples of dimethacrylates include nonanediol dimethacrylate, neopentyl glycol dimethacrylate, ethylene glycol dimethacrylate, diethylene glycol dimethacrylate, triethylene glycol dimethacrylate, polyethylene glycol dimethacrylate, etc.; triacrylates such as trimethylolpropane triacrylate, tetramethylolmethane triacrylate, pentaerythritol triacrylate, etc.; trimethacrylates such as trimethylolpropane trimethacrylate, trimethylolethane trimethacrylate, etc.; tetraacrylates such as pentaerythritol tetraacrylate, tetramethylolmethane tetraacrylate, etc.; divinyl aromatic compounds such as divinylbenzene and di-i-propenylbenzene; cyanurates such as triallyl cyanurate and triallyl isocyanurate; diallyl compounds such as diallyl phthalate; triallyl compounds: oximes such as p-quinone dioxime and p-p'-dibenzoylquinone dioxime; maleimides such as m-phenylmaleimide, and 1,2-polybutadiene.Among these, preferred are triacrylates such as diacrylate, dimethacrylate, divinyl aromatic compounds, trimethylolpropane triacrylate, tetramethylolmethane triacrylate, and pentaerythritol triacrylate; trimethacrylates such as trimethylolpropane trimethacrylate and trimethylolethane trimethacrylate; tetraacrylates such as pentaerythritol tetraacrylate and tetramethylolmethane tetraacrylate; cyanurates such as triallyl cyanurate and triallyl isocyanurate; and diallyl compounds such as diallyl phthalate; triallyl compounds: oximes such as p-quinone dioxime and p-p'-dibenzoylquinone dioxime; maleimides such as m-phenylmaleimide; and 1,2-polybutadiene, with triallyl isocyanurate being preferred.

[0120] When a crosslinking aid is used, the amount of the crosslinking aid is preferably 0.05 to 5 parts by mass, more preferably 0.2 to 4.0 parts by mass, per 100 parts by mass of copolymer (A). When the amount of the crosslinking aid is within the above range, an appropriate crosslinked structure can be achieved, improving heat resistance, mechanical properties, and adhesion. Furthermore, when a crosslinking aid is used, the mass ratio of the organic peroxide (B) to the crosslinking aid is preferably 1:10 to 10:1, more preferably 1:5 to 5:1, even more preferably 1:3 to 3:1, and particularly preferably 1:2 to 2:1. When the mass ratio is within the above range, the crosslinking reaction of the composition tends to proceed uniformly.

[0121] <Method for Producing the Resin Composition> The present composition (either the first or second embodiment) can be produced by any known method. For example, in the first embodiment, the composition can be produced by mixing a predetermined amount of copolymer (A), organic peroxide (B), silane coupling agent (C), and other components as needed, in a known method, or by mixing a predetermined amount of copolymer (A), hydrosilyl group-containing compound (D), platinum-based catalyst (E), and other components as needed, in a known method, or by melt-kneading the mixture and then granulating or grinding it.

[0122] For mixing the various components, for example, manual mixing in a bag such as a plastic bag, or mixing using a Henschel mixer, V-blender, ribbon blender, tumbler blender or the like can be employed.

[0123] Further, when melt-kneading the mixture, for example, a single-screw extruder, twin-screw extruder, kneader, Banbury mixer or the like can be used, and production with an extruder capable of continuous production is preferable. In the first embodiment, the temperature during melt-kneading is preferably 60 to 140°C, more preferably 80 to 120°C; and in the second embodiment, the temperature is preferably 30 to 130°C, more preferably 40 to 110°C.

[0124] <<Uncrosslinked Sheet>> A preferred form of the present composition (the first embodiment or the second embodiment) is a form such as a pellet form or a sheet form, more preferably a sheet form. The uncrosslinked sheet of the present invention (hereinafter also referred to as "the present uncrosslinked sheet") comprises the present composition (the first embodiment or the second embodiment). As the molding method for the present uncrosslinked sheet, various known molding methods, specifically cast molding, extrusion sheet molding, inflation molding, injection molding, compression molding and the like can be employed.

[0125] In the present specification, "uncrosslinked" means a state before crosslinking the copolymer (A) of the present invention, or a partially crosslinked state, that is, it means that the internal crosslinked structure (three-dimensional crosslinked structure) of the copolymer (A) is not sufficiently formed. In addition, in the present specification, "uncrosslinked" means that the gel fraction of the present uncrosslinked sheet measured by the following method is preferably 20% by mass or less, more preferably 10% by mass or less, still more preferably 5% by mass or less, and particularly preferably 0% by mass. (Method for measuring gel fraction) 0.10 g is collected from the present uncrosslinked sheet as a measurement sample. The measurement sample is wrapped in a 325-mesh stainless steel screen, and immersed in 30 ml of p-xylene in a sealed container at 140°C for 3 hours. Next, the screen is taken out and dried at 80°C for 2 hours or more until a constant weight is obtained. The gel fraction (% by mass) is calculated by the following formula. Gel fraction (% by mass) = 100 × (W ３ -W ２ ) / (W１ -W ２ ) (W １ : Mass of the screen and sample before immersion, W ２ : Screen mass, W ３ (Mass of the screen and sample after immersion and drying)

[0126] A preferred embodiment of the method for producing the uncrosslinked sheet involves placing the composition (first embodiment or second embodiment) containing various components, obtained by manual mixing in a bag such as a poly bag, or by mixing using an agitator such as a Henschel mixer, tumbler, or super mixer, into the hopper of an extrusion molding machine, and forming it into a sheet by extrusion while melt-kneading.

[0127] The extrusion temperature in this method is preferably 70 to 120°C. When the extrusion temperature is within this range, the occurrence of irregularities on the sheet surface due to gel generated in the extrusion molding machine can be avoided, resulting in a product appearance that tends to be good. Furthermore, when this uncrosslinked sheet is used as a sealing sheet, it tends to have good adhesion with sealing materials such as glass, solar cell elements, thin-film electrodes, and backsheets.

[0128] The thickness of this uncrosslinked sheet is typically 0.01 to 2 mm, preferably 0.05 to 1.5 mm, more preferably 0.1 to 1.2 mm, even more preferably 0.2 to 1 mm, particularly preferably 0.2 to 0.8 mm, and especially preferably 0.3 to 0.8 mm. When the thickness is within the above range, damage to glass, solar cell elements, and thin-film electrodes tends to be suppressed when this uncrosslinked sheet is used as a sealing sheet. Furthermore, when this uncrosslinked sheet is used as a sealing sheet for solar cells, the solar cell module tends to be able to secure sufficient light transmittance and increase the amount of photovoltaic power generated.

[0129] Furthermore, the surface of the uncrosslinked sheet may be embossed. Embossing improves the resistance to sheet blocking between the uncrosslinked sheets or between the uncrosslinked sheets and other sheets. Also, since embossing lowers the storage modulus of the surface of the uncrosslinked sheet, when the uncrosslinked sheet is used as a sealing sheet, it functions as a cushion for the glass, elements, and thin film electrodes when laminating the uncrosslinked sheet with the glass, elements, and thin film electrodes, thereby preventing damage to the glass, elements, and thin film electrodes.

[0130] This uncrosslinked sheet can be stored in sheet form cut to the desired size, or in a cuttable roll form. Because this uncrosslinked sheet has excellent adhesion, extrusion moldability, and crosslinkability with various materials such as glass, backsheets, thin film electrodes, aluminum, and solar cell elements, it is preferably used as a sealing sheet for batteries, and more preferably as a sealing sheet for solar cells.

[0131] One indicator of crosslinkability is the progress of crosslinking, and in some cases, the rate of increase in torque (S'Max - S'Min) (dNm) is evaluated as an indicator of the progress of crosslinking. The greater the rate of increase in torque measured under specific temperature and time conditions, the better the crosslinking reaction proceeds, and therefore it can be judged that the crosslinking is proceeding efficiently. In this invention, the rate of increase in torque of the uncrosslinked sheet is used as an indicator of the progress of crosslinking.

[0132] In the first embodiment of this composition, the torque increase of the uncrosslinked sheet measured under conditions of a temperature of 160°C and a time of 15 minutes is preferably 4.0 dNm or more, more preferably 4.5 dNm or more, even more preferably 5.0 dNm or more, and particularly preferably 5.3 dNm or more. The upper limit of the torque increase is not particularly limited, but may be 100 dNm or less. In the second embodiment of this composition, the torque increase of the uncrosslinked sheet measured under conditions of a temperature of 120°C and a time of 30 minutes is preferably 1.5 dNm or more, more preferably 2.0 dNm or more, even more preferably 2.5 dNm or more, and particularly preferably 3.0 dNm or more. The upper limit of the torque increase is not particularly limited, but may be 100 dNm or less. The torque increase (S'Max - S'Min) is determined by the method described in the examples below.

[0133] 《Crosslinked Body》 The crosslinked body of the present invention (hereinafter also referred to as "the crosslinked body") is obtained by crosslinking the composition (first embodiment or second embodiment) or the uncrosslinked sheet. The crosslinked body formed into a sheet (hereinafter also referred to as "the crosslinked sheet") has an excellent balance of mechanical strength, heat resistance, moldability and crosslinkability, and as described later, the crosslinked sheet is suitable as a encapsulant, particularly as a encapsulant for solar cells.

[0134] The crosslinked material can be manufactured, for example, by introducing the composition or the uncrosslinked sheet into a crosslinking tank (heating tank) and heating it to cause crosslinking. Depending on the application, it is preferable to pre-form the composition into the desired shape using various molding machines such as extrusion molding machines, calender rolls, press molding machines, injection molding machines, and transfer molding machines, or to crosslink it simultaneously with molding. The uncrosslinked sheet may also be pre-formed using the above-mentioned molding machines to further change its shape, depending on the application. Furthermore, molds may or may not be used during molding and / or crosslinking. If molds are not used, the composition is usually molded and crosslinked continuously.

[0135] The extrusion temperature is typically 70 to 150°C, preferably 70 to 120°C. When the extrusion temperature is within this range, there is no surface irregularity on the sheet due to gel generated in the extrusion machine during sheet forming, resulting in a good appearance. Furthermore, when voltage is applied to this crosslinked material, cracks do not occur, and the dielectric breakdown resistance tends to be good. In addition, during lamination in the manufacturing of sealing sheets, adhesion to various materials such as glass, backsheets, thin-film electrodes, aluminum, and solar cell elements tends to be good.

[0136] As for the heating method during crosslinking, known methods can be used, but various heating types such as far-infrared heating furnaces, hot air, glass bead fluidized beds, UHF (ultra-high frequency electromagnetic waves), steam, and LCM (molten salt bath) can be used. The heating conditions for the first embodiment of this composition are that the heating temperature is preferably 130 to 200°C, more preferably 140 to 160°C, and the heating time is preferably 1 to 30 minutes, more preferably 5 to 20 minutes. The heating conditions for the second embodiment of this composition are that the heating temperature is preferably 70 to 140°C, more preferably 100 to 120°C, and the heating time is preferably 1 to 30 minutes, more preferably 5 to 20 minutes.

[0137] This crosslinked material has excellent mechanical strength and heat resistance and is suitable for use in applications such as sealing materials, O-rings, industrial rolls, packing (e.g., condenser packing), gaskets, belts (e.g., heat insulating belts, copier belts, conveyor belts), hoses such as automotive hoses (e.g., water hoses, brake reservoir hoses, radiator hoses, air hoses), vibration-damping rubber, vibration-damping or vibration-reducing materials (e.g., engine mounts, motor mounts), muffler hangers, sponges (e.g., weatherstrip sponges, heat insulating sponges, protective sponges, micro-foamed sponges), cables (e.g., ignition cables, cabtyre cables, high-tension cables), wire covering materials (e.g., high-voltage wire covering materials, low-voltage wire covering materials, marine wire covering materials), glass run channels, colored surface materials, paper feed rolls, roofing sheets, and waterproof coating materials. Furthermore, by foaming this composition (first or second embodiment) simultaneously with crosslinking, it is suitable for use in applications such as shoe soles, shoe midsoles, insoles, and sandals.

[0138] 《Sealing Material》 The sealing material of the present invention (hereinafter also referred to as "this sealing material") includes this crosslinked body. A preferred embodiment of this sealing material consists solely of this crosslinked sheet.

[0139] The thickness of this sealing material is typically 0.01 to 3.0 mm, preferably 0.01 to 2.5 mm, more preferably 0.01 to 2.0 mm, even more preferably 0.01 to 1.5 mm, particularly preferably 0.01 to 1.0 mm, especially preferably 0.01 to 0.5 mm, extremely preferably 0.01 to 0.3 mm, and most preferably 0.01 to 0.2 mm. In this invention, the term "sheet" is used to include thin forms that are sometimes generally referred to as "films".

[0140] When the thickness of this encapsulant is within the aforementioned range, damage to glass, elements, and thin-film electrodes can be suppressed during the process of laminating this encapsulant onto them. Furthermore, when this encapsulant is used as an encapsulant for solar cells, solar cell modules tend to have sufficient light transmittance, thereby increasing the amount of light generated.

[0141] In the case of the present sealing material using the second embodiment of the composition, the elongation deformation rate of the present sealing material measured by the following method is preferably 5% or less, more preferably 4.5% or less, still more preferably 4.0% or less. This measurement method is an evaluation method for creep deformation, and that the elongation deformation rate falls within the above range indicates good crosslinkability and means high durability as a sealing material. (Method for measuring elongation deformation rate) The present sealing material is cut into a size of 10 mm × 70 mm to obtain a measurement sample. After attaching a double clip to one end of the measurement sample, the measurement sample is hung on a stainless steel mesh rack, a 10 g weight is hung on the other end of the measurement sample using a double clip, and the elongation deformation rate (%) after 1 hour under a condition of 90°C is measured.

[0142] The gel fraction of the present sealing material measured by the following method is preferably more than 70% by mass, more preferably more than 70% by mass and 90% by mass or less, still more preferably more than 70% by mass and 85% by mass or less. When the gel fraction exceeds the above lower limit, the crosslinkability is sufficient, and the heat resistance tends to be good when the present sealing material is used as a sealing material for solar cells. When the gel fraction is equal to or less than the above upper limit, flexibility tends to be good when used as a sealing material for solar cells. (Method for measuring gel fraction) 0.10 g of a measurement sample is collected from the present sealing material. The measurement sample is wrapped in a 325-mesh stainless steel screen, and immersed in 30 ml of p-xylene in a sealed container at 140°C for 3 hours. Next, the screen is taken out and dried at 80°C for 2 hours or more until a constant mass is reached. The gel fraction (% by mass) is calculated by the following formula. Gel fraction (% by mass) = 100 × (W ３ -W ２ ) / (W １ -W ２ ) (W １ : mass of the screen and the measurement sample before immersion, W ２ : mass of the screen, W ３ : mass of the screen and the measurement sample after immersion and drying)

[0143] This encapsulant has excellent mechanical strength and heat resistance and is suitable for use in semiconductor packages such as IC chips (integrated circuits), transistors, and diodes; capacitors such as LEDs (light-emitting diodes), electrolytic capacitors, and film capacitors; sensors such as pressure sensors, temperature sensors, and acceleration sensors; batteries such as solar cells, lithium-ion batteries, and secondary batteries; optical components such as printed circuit boards (PCBs), MEMS devices (microelectromechanical systems), camera modules, and optical fiber connectors; automotive electronic components such as ECUs (electronic control units), sensor modules, and ignition coils; and medical devices such as implantable devices and internal sensors. Among these, it is preferably used as an encapsulant for batteries, and more preferably as an encapsulant for solar cells.

[0144] <Method for Manufacturing the Sealing Material> The sealing material is preferably manufactured by the same method as the crosslinked body described above. The preferred form of the sealing material is a sheet (hereinafter also referred to as "the sealing sheet").

[0145] The sealing sheet preferably includes the crosslinked sheet, and more preferably includes at least one layer made of the crosslinked sheet. When the sealing sheet includes at least one layer made of the crosslinked sheet, there may be one or two or more layers of the crosslinked sheet. When the sealing sheet is used as a sealing material for solar cells, it is also preferable for the crosslinked sheet to be a single layer, from the viewpoint of simplifying the structure and reducing costs, and from the viewpoint of minimizing inter-layer interface reflection and effectively utilizing light.

[0146] Furthermore, the sealing sheet may consist only of a layer made of the crosslinked sheet, or it may have layers other than the crosslinked sheet (hereinafter also referred to as "other layers"). Examples of other layers, if classified by purpose, include hard coat layers for surface or back surface protection, adhesive layers, anti-reflective layers, gas barrier layers, anti-fouling layers, etc. Examples of other layers, if classified by material, include layers made of ultraviolet-curable resins, thermosetting resins, polyolefin resins, carboxylic acid-modified polyolefin resins, fluorine-containing resins, cyclic olefin (co)polymers, inorganic compounds, etc.

[0147] If the sealing sheet has other layers, there are no particular restrictions on the positional relationship between the layers made of the crosslinked sheet and the other layers, and a preferred layer configuration can be appropriately selected in relation to the objectives of the present invention. When the sealing sheet is used as a sealing material for solar cells, the other layers may be provided between two or more layers made of the crosslinked sheet, on the outermost layer of the sealing sheet, or at any other location. Furthermore, the other layers may be provided on only one side of the layers made of the crosslinked sheet, or on both sides. There are no particular restrictions on the number of other layers; any number of other layers may be provided, or no other layers may be provided at all.

[0148] When using this sealing sheet as a sealing material for solar cells, from the viewpoint of simplifying the structure and reducing costs, and from the viewpoint of minimizing interfacial reflection and effectively utilizing light, it is preferable to manufacture the sealing sheet using only a layer made of this crosslinked sheet without providing any other layers; in other words, it is preferable that the sealing sheet be composed only of a layer made of this crosslinked sheet. However, if there are other layers that are necessary or useful in relation to the objectives of the present invention, those other layers may be provided as appropriate. When other layers are provided, there are no particular restrictions on the method of laminating layers made of this crosslinked sheet with each other, with the layers made of this crosslinked sheet and other layers, or with other layers, but it is preferable to obtain a laminate by co-extruding using a known melt extruder such as a cast molding machine, extruded sheet molding machine, inflation molding machine, or injection molding machine, or by melting or heat laminating one layer onto one layer that has been pre-formed to obtain a laminate.

[0149] Furthermore, layers may be laminated between each layer by dry lamination or heat lamination using an adhesive layer, as needed. Known adhesives can be used, such as maleic anhydride-modified polyolefin resins (e.g., "Admer" from Mitsui Chemicals, Inc., "Modic" from Mitsubishi Chemical Corporation); low (non)crystalline soft polymers such as unsaturated polyolefins; acrylic adhesives such as ethylene / acrylic acid ester / maleic anhydride ternary copolymers (e.g., "BONDINE" from Arkema Corporation); ethylene / vinyl acetate copolymers; polyester adhesives; polyurethane adhesives; or adhesive resin compositions containing these. Adhesives with heat resistance of approximately 120 to 150°C are preferred, and examples include polyester or polyurethane adhesives. Additionally, to improve interlayer adhesion, treatments such as silane coupling treatment, titanium coupling treatment, corona treatment, or plasma treatment may be applied to the layers.

[0150] 《Solar Cell Module》 The solar cell module of the present invention (hereinafter also referred to as "this solar cell module") includes, for example, a crystalline solar cell module in which solar cell elements formed from polycrystalline silicon or the like are sandwiched and laminated with this encapsulating material (preferably this encapsulating sheet), and both the front and back surfaces are further covered with protective sheets. That is, for example, this solar cell module has a configuration of: protective sheet for solar cell module (front protective member) / encapsulating layer containing this encapsulating material / solar cell element (crystalline solar cell element containing monocrystalline silicon) / encapsulating sheet / protective sheet for solar cell module (back protective member).

[0151] One embodiment of this solar cell module is a solar cell module comprising a transparent protective member on the front side, a protective member on the back side, a solar cell element, and a sealing layer containing the sealing material that seals the solar cell element between the transparent protective member on the front side and the protective member on the back side.

[0152] It should be noted that the preferred embodiment of this solar cell module is not limited to the above configuration, and some of the above components may be omitted or other layers or components may be provided as appropriate, as long as the objective of the present invention is not impaired. Examples of other layers or components include adhesive layers (adhesive members), shock-absorbing layers (shock-absorbing members), coating layers (coating members), anti-reflective layers (anti-reflective members), back-surface reflective layers (back-surface reflective members), and light-diffusing layers (light-diffusing members). These layers or components are not particularly limited, but they may be provided in appropriate positions considering the purpose and characteristics of each layer or component.

[0153] <Method for Manufacturing a Solar Cell Module> The method for manufacturing this solar cell module includes, for example, (i) a step of stacking a transparent protective member on the front side, the uncrosslinked sheet, a solar cell element (cell), the uncrosslinked sheet, and the protective member on the back side in this order to form a laminate, and (ii) a step of pressing and heating the obtained laminate to integrate it.

[0154] In step (i), if an embossed shape is formed on the surface of the uncrosslinked sheet, it is preferable to position it so that this surface faces the solar cell element. In step (ii), the laminate obtained in step (i) is heated and pressurized using a vacuum laminator or a hot press according to a conventional method to integrate (seal) it. During the sealing operation, the uncrosslinked sheet has high cushioning properties, which prevents damage to the solar cell element. In addition, because it has good degassing properties, there is no air entrapment, and high-quality products can be manufactured with a good yield.

[0155] During the manufacturing of the solar cell module, the uncrosslinked sheet is crosslinked. This crosslinking process may be performed simultaneously with or after process (ii). The crosslinking process performed after process (ii) can be carried out by a general method, for example, a tunnel-type continuous crosslinking furnace or a tray-type batch crosslinking furnace may be used.

[0156] When the crosslinking process is performed after step (ii), in the uncrosslinked sheet including the first embodiment of the composition, for example, in step (ii), the sheet is vacuum-heated for 3 to 6 minutes under conditions of a heating temperature of 125 to 160°C and a vacuum pressure of 10 Torr or less; then pressurized by atmospheric pressure for about 1 to 15 minutes to integrate the laminate. The crosslinking conditions for the crosslinking process performed after step (ii) are preferably 130 to 200°C, more preferably 140 to 160°C, and preferably 1 to 30 minutes, more preferably 5 to 20 minutes. Furthermore, in the uncrosslinked sheet including the second embodiment of the composition, for example, in step (ii), the sheet is vacuum-heated for 3 to 6 minutes under conditions of a heating temperature of 130°C or less, preferably 125°C or less and a vacuum pressure of 10 Torr or less; then pressurized by atmospheric pressure for about 1 to 15 minutes to integrate the laminate. The crosslinking conditions for the crosslinking step performed after step (ii) are preferably 70 to 140°C, more preferably 100 to 120°C, and preferably 1 to 30 minutes, more preferably 5 to 20 minutes.

[0157] On the other hand, when the crosslinking process is performed simultaneously with process (ii), in the uncrosslinked sheet including the first embodiment of the composition, the crosslinking process can be carried out in the same manner as when it is performed after process (ii), except that the heating temperature in process (ii) is set to 70 to 160°C, preferably 75 to 155°C, and the pressurization time by atmospheric pressure is set to 6 to 30 minutes. Furthermore, in the uncrosslinked sheet including the second embodiment of the composition, the crosslinking process can be carried out in the same manner as when it is performed after process (ii), except that the heating temperature in process (ii) is set to 70 to 130°C, preferably 75 to 125°C, and the pressurization time by atmospheric pressure is set to 6 to 30 minutes. The first embodiment of this composition contains a specific organic peroxide (B), and the second embodiment contains a specific hydrosilyl group-containing compound, both exhibiting excellent crosslinking properties. Since step (ii) does not require a two-step bonding process and can be completed in a short time at a high temperature, the crosslinking process performed after step (ii) may be omitted, significantly improving the productivity of the module.

[0158] In the manufacturing of this solar cell module, it is preferable to suppress the decomposition of the crosslinking agent and temporarily adhere the uncrosslinked sheet to the solar cell elements and protective material at a temperature at which the uncrosslinked sheet melts, and then raise the temperature of the laminate to simultaneously achieve sufficient adhesion and crosslinking of the uncrosslinked sheet. The additives (other components mentioned above) contained in the uncrosslinked sheet may be appropriately selected in a formulation that satisfies all conditions.

[0159] The gel fraction of the solar cell module, as measured by the following method, is preferably 50 to 95%, more preferably 50 to 90% by mass, even more preferably 60 to 90% by mass, and particularly preferably 60 to 85% by mass. If the gel fraction is above the lower limit, the heat resistance of the encapsulant in the solar cell module is good. If the gel fraction is below the upper limit, the encapsulant in the solar cell module is good. (Method for measuring gel fraction) 1 g of encapsulant is taken from the solar cell module as a measurement sample. The measurement sample is extracted with p-xylene at 140°C for 3 hours, filtered through a 325 mesh stainless steel mesh, and then the mesh is dried under reduced pressure at 80°C for 2 hours or more. The gel fraction (remaining amount / mass of encapsulant sheet sample) is calculated from the remaining amount on the mesh (mass%).

[0160] This solar cell module can be used in various types of solar cells. Specifically, examples include perovskite solar cells containing a solar cell element (power generation layer) containing a perovskite compound, perovskite-silicon tandem solar cells combining a solar cell element containing a perovskite compound and a crystalline solar cell element containing single-crystal silicon, lightweight and easy-to-handle organic thin-film solar cells, flexible solar cells prioritizing cost reduction and design aesthetics, and solar cells with transparent resin or film applied to a light-transmitting substrate. Among these, the encapsulant including the second embodiment of this composition is suitable for solar cell modules containing one or more perovskite compounds in the solar cell element. Perovskite compounds are known to be sensitive to heat, and with the second embodiment of this composition, it is expected that the crosslinking reaction will proceed at a temperature at which the perovskite compound does not decompose.

[0161] The present invention will be described in more detail below based on examples, but the present invention is not limited to these examples. In the following description, unless otherwise specified, "parts" refers to "parts by mass".

[0162] [Example 1A] Synthesis of ethylene-1-butene-VNB copolymer (A-1) Using a 2 L stainless steel autoclave equipped with a stirring blade, the polymerization reaction of ethylene, 1-butene, and 5-vinyl-2-norbornene (VNB) was carried out continuously at 87°C. Hexane was used as the polymerization solvent and was continuously supplied to the polymerizer at a rate of ethylene feed of 125 g / h, 1-butene feed of 258 g / h, VNB feed of 2.6 g / h, and hydrogen feed of 2.9 NL / h. While maintaining the polymerization pressure at 1.6 MPaG and the polymerization temperature at 87°C, di(p-tolyl)methylene(cyclopentadienyl)(octamethyloctahydrodibenzofluorenyl)zirconium dichloride was used as the main catalyst and continuously supplied to the polymerizer at a feed rate of 0.0009 mmol / h. Furthermore, methyl aluminoxane was continuously supplied to the polymerizer at a feed rate of 0.41 mmol / h as a co-catalyst, and triisobutylaluminum was continuously supplied to the polymerizer at a feed rate of 1.0 mmol / h as an organoaluminum compound. In this way, a solution containing ethylene-1-butene-VNB copolymer formed from ethylene, 1-butene, and VNB was obtained. A small amount of methanol was added to the polymerization reaction solution withdrawn from the bottom of the polymerizer to stop the polymerization reaction, and the ethylene-1-butene-VNB copolymer was separated from the solvent by steam stripping. The resulting material was then passed through a twin-screw extruder and cut into pellets at the extruder tip with a pellet cutter to obtain ethylene-1-butene-VNB copolymer (A-1) as pellets. The obtained ethylene-1-butene-VNB copolymer (A-1) was dried under reduced pressure at 80°C overnight. Through the above operations, ethylene-1-butene-VNB copolymer (A-1) (hereinafter also referred to as "polymer (A-1)") was obtained.

[0163] [Example 2A] Synthesis of ethylene-1-butene-VNB copolymer (A-2) A 130 L polymerizer equipped with a stirring blade was used to continuously polymerize ethylene, 1-butene, and VNB at 87°C. Hexane was used as the polymerization solvent and was continuously supplied to the polymerizer at a rate of 7.30 kg / h for ethylene, 5.49 kg / h for 1-butene, 200 g / h for VNB, and 328 NL / h for hydrogen. While maintaining a polymerization pressure of 1.6 MPaG and a polymerization temperature of 87°C, di(p-tolyl)methylene(cyclopentadienyl)(octamethyloctahydrodibenzofluorenyl)zirconium dichloride was used as the main catalyst and continuously supplied to the polymerizer at a feed rate of 0.01 mmol / h. Furthermore, methyl aluminoxane was continuously supplied to the polymerizer at a feed rate of 4.25 mmol / h as a co-catalyst, and triisobutylaluminum was continuously supplied to the polymerizer at a feed rate of 15.0 mmol / h as an organoaluminum compound. In this way, a solution containing ethylene-1-butene-VNB copolymer formed from ethylene, 1-butene, and VNB was obtained. A small amount of methanol was added to the polymerization reaction solution withdrawn from the bottom of the polymerizer to stop the polymerization reaction, and the ethylene-1-butene-VNB copolymer was separated from the solvent by steam stripping. The resulting material was then passed through a twin-screw extruder and cut into pellets at the extruder tip with a pellet cutter to obtain ethylene-1-butene-VNB copolymer (A-2) as pellets. The obtained ethylene-1-butene-VNB copolymer (A-2) was dried under reduced pressure at 80°C overnight. Through these operations, ethylene-1-butene-VNB copolymer (A-2) (hereinafter also referred to as "polymer (A-2)") was obtained at a rate of 7.7 kg per hour.

[0164] [Example 3A] The ethylene-1-butene-VNB copolymer (A-3) was obtained at a rate of 8.5 kg per hour, in the same manner as in Example 2A, except that the ethylene feed amount was 7.01 kg / h, the 1-butene amount was 5.83 kg / h, the VNB feed amount was 300 g / h, and the hydrogen feed amount was 263 NL / h.

[0165] [Example 4A] The ethylene-1-butene-VNB copolymer (A-4) was produced in the same manner as in Example 2A, except that the ethylene feed amount was 7.00 kg / h, the 1-butene amount was 5.55 kg / h, the VNB feed amount was 400 g / h, and the hydrogen feed amount was 309 NL / h. The ethylene-1-butene-VNB copolymer (A-4) (hereinafter referred to as "polymer (A-4)") was obtained at a rate of 7.8 kg per hour.

[0166] [Example 5A] The ethylene-1-butene-VNB copolymer (A-5) was synthesized in the same manner as in Example 2A, except that the ethylene feed amount was 7.30 kg / h, the 1-butene amount was 6.01 kg / h, the VNB feed amount was 200 g / h, and the hydrogen feed amount was 130 NL / h. The ethylene-1-butene-VNB copolymer (A-5) (hereinafter also referred to as "polymer (A-5)") was obtained at a rate of 7.5 kg per hour. The physical properties of the obtained copolymer (A-5) were measured by the method described above.

[0167] [Comparative Example 1A] A polymerization reaction of ethylene, propylene, and VNB was carried out continuously at 110°C using a 300 L polymerizer equipped with a synthetic stirring blade for the ethylene-propylene-VNB copolymer (a-1). Hexane was used as the polymerization solvent and was continuously supplied to the polymerizer at a rate of 4.7 kg / h for ethylene, 4.3 kg / h for propylene, 240 g / h for VNB, and 220 NL / h for hydrogen. While maintaining a polymerization pressure of 1.7 MPaG and a polymerization temperature of 110°C, di(p-tolyl)methylene(cyclopentadienyl)(octamethyloctahydrodibenzofluorenyl)zirconium dichloride was used as the main catalyst and continuously supplied to the polymerizer at a feed rate of 0.015 mmol / h. Furthermore, (C6H5)3CB(C6F5)4 was continuously supplied to the polymerizer at a feed rate of 0.075 mmol / h as a co-catalyst, and triisobutylaluminum was continuously supplied at a feed rate of 20 mmol / h as an organoaluminum compound. In this way, a solution containing an ethylene-propylene-VNB copolymer formed from ethylene, propylene, and VNB was obtained. A small amount of methanol was added to the polymerization reaction solution withdrawn from the bottom of the polymerizer to stop the polymerization reaction, and the ethylene-1-butene-VNB copolymer was separated from the solvent by steam stripping. The resulting material was then passed through a twin-screw extruder and cut into pellets with a pellet cutter at the tip of the extruder to obtain ethylene-1-butene-VNB copolymer (a-1) as pellets. The obtained ethylene-1-butene-VNB copolymer (a-1) was dried under reduced pressure at 80°C overnight. Through the above operations, ethylene-propylene-VNB copolymer (a-1) (hereinafter also referred to as "polymer (a-1)") was obtained.

[0168] [Comparative Example 2A] Synthesis of ethylene-1-butene-VNB copolymer (a-2) A 300 L polymerizer equipped with a stirring blade was used to continuously polymerize ethylene, 1-butene, and VNB at 95°C. Hexane was used as the polymerization solvent and was continuously supplied to the polymerizer at a rate of 5.3 kg / h for ethylene, 21.5 kg / h for 1-butene, 566 g / h for VNB, and 10 NL / h for hydrogen. While maintaining a polymerization pressure of 1.6 MPaG and a polymerization temperature of 95°C, di(p-tolyl)methylene(cyclopentadienyl)(octamethyloctahydrodibenzofluorenyl)zirconium dichloride was used as the main catalyst and continuously supplied to the polymerizer at a feed rate of 0.00903 mmol / h. Furthermore, (C6H5)3CB(C6F5)4 was continuously supplied to the polymerizer at a feed rate of 0.045 mmol / h as a co-catalyst, and triisobutylaluminum was continuously supplied at a feed rate of 30 mmol / h as an organoaluminum compound. In this way, a solution containing ethylene-1-butene-VNB copolymer formed from ethylene, 1-butene, and VNB was obtained. A small amount of methanol was added to the polymerization reaction solution withdrawn from the bottom of the polymerizer to stop the polymerization reaction, and the ethylene-1-butene-VNB copolymer was separated from the solvent by steam stripping. The resulting material was then passed through a twin-screw extruder and cut into pellets at the extruder tip with a pellet cutter to obtain ethylene-1-butene-VNB copolymer (a-2) as pellets. The obtained ethylene-1-butene-VNB copolymer (a-2) was dried under reduced pressure at 80°C overnight. Through the above operations, ethylene-1-butene-VNB copolymer (a-2) (hereinafter also referred to as "polymer (a-2)") was obtained.

[0169] [Comparative Example 3A] Synthesis of ethylene-1-butene-VNB copolymer (a-3) A polymerizer with a volume of 130 L equipped with a stirring blade was used to continuously carry out the polymerization reaction of ethylene, 1-butene, and VNB at 115°C. Hexane was used as the polymerization solvent and was continuously supplied to the polymerizer at a rate of 8.1 kg / h for ethylene, 9.4 kg / h for 1-butene, 50.1 g / h for VNB, and 375 NL / h for hydrogen. While maintaining a polymerization pressure of 3.3 MPaG and a polymerization temperature of 115°C, di(p-tolyl)methylene(cyclopentadienyl)(octamethyloctahydrodibenzofluorenyl)zirconium dichloride was used as the main catalyst and continuously supplied to the polymerizer at a feed rate of 0.0042 mmol / h. Furthermore, methyl aluminoxane was continuously supplied to the polymerizer at a feed rate of 2.23 mmol / h as a co-catalyst, and triisobutylaluminum was continuously supplied to the polymerizer at a feed rate of 3.0 mmol / h as an organoaluminum compound. In this way, a solution containing ethylene-1-butene-VNB copolymer formed from ethylene, 1-butene, and VNB was obtained. A small amount of methanol was added to the polymerization reaction solution withdrawn from the bottom of the polymerizer to stop the polymerization reaction, and the ethylene-1-butene-VNB copolymer was separated from the solvent by steam stripping. The mixture was then passed through a twin-screw extruder and cut into pellets with a pellet cutter at the tip of the extruder to obtain ethylene-1-butene-VNB copolymer (a-3) as pellets. The obtained ethylene-1-butene-VNB copolymer (a-3) was dried under reduced pressure at 80°C for 24 hours. Through the above operations, ethylene-1-butene-VNB copolymer (a-3) (hereinafter also referred to as "polymer (a-3)") was obtained.

[0170] [Comparative Example 4A] Synthesis of ethylene-propylene-VNB copolymer (a-4) 1030 mL of hexane and 5.4 mL of VNB were charged into a 2 L stainless steel autoclave that had been thoroughly nitrogen-purged. After raising the temperature of the system to 160°C, propylene was charged at a partial pressure of 0.91 MPa, and ethylene was supplied to bring the total pressure to 2.4 MPaG. Next, 0.3 mmol of triisobutylaluminum, 0.00012 mmol of di(p-tolyl)methylene(cyclopentadienyl)(octamethyloctahydrodibenzofluorenyl)zirconium dichloride and 0.0012 mmol of triphenylcarbeniumtetrakis(pentafluorophenyl)borate were injected under pressure with nitrogen, and polymerization was started by increasing the stirring speed to 250 rpm. Thereafter, the total pressure was maintained at 2.4 MPa-G by continuously supplying only ethylene, and polymerization was carried out at 160°C for 10 minutes. Polymerization was stopped by adding a small amount of methanol to the system, and then unreacted ethylene was purged. The resulting polymer solution was added to a large excess methanol / acetone mixture, air-dried overnight, and the resulting polymer was recovered by filtration. It was then dried overnight under reduced pressure at 130°C to obtain 11.04 g of ethylene-propylene-VNB copolymer (a-4) (hereinafter also referred to as "polymer (a-4)").

[0171] [Measurement and Evaluation Methods for Ethylene-α-Olefin-Non-Conjugated Polyene Copolymers, etc.] The physical properties and characteristics of ethylene-α-olefin-non-conjugated polyene copolymers, etc. obtained in the examples and comparative examples were measured by the following methods. The results are shown in Table 1.

[0172] <Content of Each Constituent Unit> The content (mol%) of each structural unit constituting the ethylene-α-olefin-non-conjugated polyene copolymers synthesized in Examples 1A to 5A and Comparative Examples 1A to 4A was determined by intensity measurement using a nuclear magnetic resonance spectrometer by the following method. Specifically, o-dichlorobenzene-d ４ The measurement was performed using the solvent at a temperature of 120°C, with a spectral width of 20 ppm, a pulse repetition time of 7.0 seconds, and a pulse width of 6.15 μsec (45° pulse). The results obtained were then obtained. １ H-NMR spectrum or １３The molar amount (mol%) of each structural unit was calculated based on the cumulative value of the relevant peaks observed in the 1C spectrum. The calculated content (mol%) was rounded to two decimal places. (Measurement conditions) Apparatus: ECX400P nuclear magnetic resonance spectrometer manufactured by JEOL Ltd. Measurement nuclei: 1H (400 MHz); 13C (125 MHz) Measurement mode: Single pulse Pulse width: 45° (5.25 μsec) Number of points: 32 k Measurement range: 20 ppm (-4 to 16 ppm) Repetition time: 7.0 sec Number of integrations: 64 Measurement solvent: Orthodichlorobenzene-d ４ Sample concentration: ca. 20 mg / 0.6 mL; Measurement temperature: 120°C; Window function: exponential (BF: 0.12 Hz); Chemical shift reference: orthodichlorobenzene (7.1 ppm)

[0173] <Glass Transition Temperature (Tg)> The glass transition temperature (Tg) of the ethylene-α-olefin-non-conjugated polyene copolymers synthesized in Examples 1A to 5A and Comparative Examples 1A to 4A was determined by DSC measurement under the following conditions. Using a differential scanning calorimeter (X-DSC7000, manufactured by SII), approximately 10 mg of the sample was heated from 30°C to 200°C at a heating rate of 50°C / min in a nitrogen atmosphere and held at that temperature for 10 minutes. It was then cooled to -90°C at a cooling rate of 10°C / min and held at that temperature for 1 minute, after which it was heated to 150°C at a heating rate of 10°C / min.

[0174] <Melt Flow Rate (MFR): MFR ２ MFR １０ MFR １０ / MFR ２ > The melt flow rates of ethylene-α-olefin-non-conjugated polyene copolymers synthesized in Examples 1A to 5A and Comparative Examples 1A and 3A were subjected to MFR testing at a temperature of 190°C under loads of 2.16 kg and 10 kg, in accordance with ASTM D1238E. ２ (g / 10 min) and MFR １０ Calculate (g / 10 min) for each, and from these values, calculate MFR １０ / MFR ２ The value was calculated.

[0175] <Pellet Handling Properties> 100 g of pellets of ethylene-α-olefin-non-conjugated polyene copolymer, etc., synthesized in Examples 1A to 5A and Comparative Examples 1A to 4A, were packed into a polybag measuring 90 mm in length and 90 mm in width. A 10 kg load was applied to the sample, and it was stored at 50°C for 3 days. The pellet blocking force and the way the pellet aggregate collapsed after the test were evaluated using a push-pull gauge. The way the pellet aggregate collapsed after the test was judged visually according to the following criteria: A: The copolymer forming the pellet aggregate collapses while maintaining its pellet shape, or some of the pellet aggregate collapses while maintaining its pellet shape, and some remain fixed. B: The pellets are completely fixed together and do not collapse.

[0176] <Sheet Blocking Resistance> Ethylene-α-olefin-non-conjugated polyene copolymers synthesized in Examples 1A to 5A and Comparative Examples 1A to 3A were used to form 0.5 mm thick sheets at a gauge pressure of 10 MPa using a hydraulic hot press (NS-50) manufactured by Shinto Metal Industries Co., Ltd., set to 100°C. Strips measuring 3 cm x 12 cm were cut from the obtained sheets and used as measurement samples. Only the 4 cm portion from the edge was bonded together, and a 500 g weight was placed on the bonded portion of the laminated sheet. After standing in a 40°C oven for 24 hours, the sheet was removed and cooled at room temperature for 30 minutes, and the peel strength of the sheet was measured. The peel test was performed using a peel test apparatus (EMX-500N and Push-Plug Gauge manufactured by Imada Co., Ltd.) with a 180° peel between sheets, under conditions of a span of 12 cm, a tensile speed of 300 mm / min, and 23°C. The average of three measurements was used to evaluate sheet blocking resistance according to the following criteria. In Table 1, "resin strength" refers to the strength (N / cm) at which the resin breaks during the tensile test in the peel test described above. A: Since "peel strength ≤ resin strength", it is possible to measure the peel strength. B: Since "peel strength > resin strength", it is impossible to measure the peel strength. In this case, in Table 1, the evaluation of "resin strength" is set to "resin breakage" because it is impossible to measure the peel strength.

[0177]

[0178] As shown in Table 1, the ethylene-α-olefin-non-conjugated polyene copolymers of Examples 1A to 5A exhibit superior sheet blocking resistance compared to the ethylene-α-olefin-non-conjugated polyene copolymers of Comparative Examples 1A to 2A. Furthermore, the ethylene-α-olefin-non-conjugated polyene copolymers of Examples 1A to 5A also exhibit superior pellet handling properties compared to the ethylene-α-olefin-non-conjugated polyene copolymers of Comparative Examples 1A to 2A.

[0179] [Examples 1B to 5B, Comparative Examples 1B and 2B] To 100 parts by mass of the ethylene-α-olefin-non-conjugated polyene copolymer synthesized in Examples 1A to 5A, Comparative Example 1A and Comparative Example 3A, 0.7 parts by mass of tert-butylperoxy-2-ethylhexyl carbonate with a 1-minute half-life temperature of 161°C was added as the organic peroxide (B), 0.2 parts by mass of γ-methacryloxypropyltrimethoxysilane was added as the silane coupling agent (C), and 0.1 parts by mass of bis(2,2,6,6-tetramethyl-4-piperidyl) sebacate was added as the weather stabilizer. The resulting mixtures were melt-kneaded using a Laboplast Mill (twin-screw batch type melt-kneading device) manufactured by Toyo Seiki Co., Ltd. at 90°C, screw rotation speed: 30 rpm, and kneading time: 5 minutes to obtain resin compositions 1-1 to 1-7, respectively.

[0180] [Measurement and Evaluation Method of Resin Compositions] The crosslinking properties were evaluated using resin compositions 1-1 to 1-7 obtained in Examples 1B to 5B, Comparative Example 1B, and Comparative Example 2B. The results are shown in Table 2.

[0181] <Crosslinking Properties (Increase in Torque (S'Max - S'Min))> Using resin compositions 1-1 to 1-7 obtained in Examples 1B to 5B, Comparative Example 1B, and Comparative Example 2B, a curometer test was performed using a measuring device: MDR2000P (manufactured by ALPHA TECHNOLOGIES) under measurement conditions of a temperature of 160°C and a time of 15 minutes, and the increase in torque (S'Max - S'Min) (dNm) was measured as follows. A sample was set in the measuring device, and the torque change obtained under constant temperature and constant shear rate conditions was measured to obtain a vulcanization curve. From this vulcanization curve, the minimum torque value S'Min (dNm) and the maximum torque value S'Max (dNm) were determined, and the progress of crosslinking was confirmed by the increase in torque (S'Max - S'Min).

[0182]

[0183] As shown in Table 2, the resin compositions of Examples 1B to 5B exhibit a greater increase in torque and superior crosslinking properties (crosslinkability) compared to the resin compositions of Comparative Examples 1B and 2B.

[0184] [Synthesis Example 1] 536 g of methylhydrogenpolysiloxane represented by the following formula (B1b) was charged into a reactor for the synthesis of hydrosilyl group-containing compound (D-1), and heated to 40°C while stirring under a nitrogen flow. 0.4 g of a toluene solution of platinum-1,3,5,7-tetravinyl-1,3,5,7-tetramethylcyclotetrasiloxane complex (Pt concentration 0.3 wt%) was added, and 265 g of α-methylstyrene was added dropwise while maintaining the reaction temperature at 40-90°C. After the dropwise addition was completed, stirring was continued at 85°C for 2 hours, and then 0.5 g of the reaction solution was taken, and the reaction rate of the Si-H groups was confirmed to be approximately 36% by the alkaline decomposition gas generation method (decomposing the remaining Si-H groups with an ethanol / aqueous solution of KOH, and calculating the reaction rate of the Si-H groups from the volume of hydrogen gas generated). Next, the reaction mixture was heated under reduced pressure to 135°C and the low-boiling components were distilled off for 2 hours to obtain 673 g of the hydrosilyl group-containing compound (B-1). The obtained compound (B-1) was, ２９Si-NMR confirmed that the compound was represented by the following formula (B1a). The viscosity of the obtained hydrosilyl group-containing compound (D-1) was measured at 25°C using an Ubbelohde-type viscosity tube in accordance with JIS Z 8803:2011, and was found to be 26 mmHg. ２ It was / s.

[0185]

[0186] [Synthesis Example 2] Synthesis of Adhesion-Enhancing Agent (G-1) A resin that will be the main component of the silane-modified resin was produced by the method described below. Using a stainless steel polymerization reactor with an internal volume of 130 L equipped with stirring blades, copolymerization of ethylene and 1-butene was carried out continuously at a polymerization temperature of 115°C and a polymerization pressure of 3.3 MPaG (MPa gauge pressure). Dehydrated and purified hexane was continuously supplied from the side of the polymerization reactor at a rate of 9.1 L per hour, ethylene at a rate of 6.5 kg, 1-butene at a rate of 7.8 kg, hydrogen at a rate of 200 NL, di(p-tolyl)methylene(cyclopentadienyl)(octamethyloctahydrodibenzofluorenyl)zirconium dichloride at a rate of 0.027 mmol, methylaluminoxane at a rate of 2.0 mmol, and triisobutylaluminum at a rate of 1.5 mmol to carry out the copolymerization reaction. The hexane solution of the generated ethylene-1-butene copolymer was continuously discharged through an outlet provided on the side wall of the polymerizer. The obtained hexane solution of ethylene-1-butene copolymer was introduced into a heater and heated to 180°C. 80 mL of methanol was added per hour as a catalyst deactivator to stop polymerization, and the solution was continuously transferred to a defloration process under reduced pressure and dried to obtain ethylene-1-butene copolymer (g-1), which is the main component resin. The obtained ethylene-1-butene copolymer (g-1) had a 1-butene content of 14.9 mol%, an MFR (According to ASTM D1238E, 190°C, 2.16 kg load) of 3.6 g / 10 min, and a yield of 7.5 kg per hour. To the ethylene-1-butene copolymer (g-1) obtained by the above method, 0.5 parts by mass of γ-methacryloxypropyltrimethoxysilane and 0.09 parts by mass of 2,5-dimethyl-2,5-bis(tert-butylperoxy)hexine were added and dry-blended to obtain a blend of ethylene-1-butene copolymer (g-1). Next, using a Laboplast Mill manufactured by Toyo Seiki Seisakusho Co., Ltd., the obtained ethylene copolymer blend was melt-kneaded at 200°C and 40 rpm for 5 minutes to obtain an adhesion promoter (G-1), which is a silane-modified resin of ethylene-1-butene copolymer. The adhesion promoter (G-1) had a graft Si content of 0.04 wt% and an MFR (according to ASTM D1238E, 190°C, 2.16 kg load) of 1.0 g / 10 min.

[0187] [Example 1C] Per 100 parts by mass of copolymer (A-2), 3.0 parts by mass of hydrosilyl group-containing compound (D-1) as hydrosilyl group-containing compound (D), 0.2 parts by mass of SRX212Catalist (manufactured by Dow Toray Ltd., a product containing 1% to less than 3% by mass of 1,1,3,3-tetramethyl-1,3-divinyldisiloxane platinum complex) as platinum catalyst (E), and 1-ethynylcyclohexane as reaction inhibitor (F). Xanol (manufactured by Nisshin Chemical Industry Co., Ltd.) was added in an amount of 0.1 parts by mass, γ-methacryloxypropyltrimethoxysilane (manufactured by Shin-Etsu Chemical Co., Ltd., KBM-530) as a silane coupling agent (C) was added in an amount of 0.2 parts by mass, and bis(2,2,6,6-tetramethylpiperidine-4-yl)decandioate (manufactured by BASF Japan Ltd., Tinuvin 770) as a weather-resistant stabilizer was added in an amount of 0.1 parts by mass. The resulting mixture was melt-kneaded using a 6-inch roll at a kneading temperature of 60°C to obtain resin composition 2-1. The kneading conditions were as follows: roll temperature front roll / rear roll = 60°C / 60°C, roll peripheral speed front roll / rear roll = 18 rpm / 15 rpm, roll gap = 2 mm, and kneading time 60 minutes. The obtained resin composition 2-1 was molded for 2 minutes under a pressure of 10 MPa after preheating for 5 minutes using a hydraulic hot press machine set to 90°C, and then cooled for 4 minutes under a pressure of 10 MPa at 20°C to produce an uncrosslinked sheet 2-1 measuring 60 mm x 100 mm with a thickness of 0.5 mm. The obtained uncrosslinked sheet 2-1 was placed in a vacuum laminator (NPC Corporation, LM-110X160S), placed on a hot plate heated to 120°C, and subjected to reduced pressure for 5 minutes and heating for 15 minutes to produce a crosslinked sheet 2-1 with a thickness of 0.5 mm.

[0188] [Example 2C] Resin composition 2-2, uncrosslinked sheet 2-2, and crosslinked sheet 2-2 were prepared in the same manner as in Example 1C, except that the silane coupling agent (C) was not included, 25 parts by mass of adhesion promoter (G-1) was included as adhesion promoter (G) (relative to 100 parts by mass of copolymer (A-2)), the amount of platinum-based catalyst (E) was changed to 0.05 parts by mass, and the amount of reaction inhibitor (F) was changed to 0.05 parts by mass.

[0189] [Examples 3C to 4C] Resin compositions 2-3 to 2-4, uncrosslinked sheets 2-3 to 2-4, and crosslinked sheets 2-3 to 2-4 were prepared in the same manner as in Example 2C, except that copolymer (A-2) was changed to the copolymer species listed in Table 3.

[0190] [Measurement and Evaluation Methods for Resin Compositions and Crosslinked Sheets] The crosslinking properties were evaluated using the resin compositions obtained in Examples 1C to 4C. In addition, the glass adhesion properties were evaluated using the uncrosslinked sheets obtained in Examples 1C to 4C. Furthermore, the gel fraction, light transmittance, volume resistivity, and creep (extensional deformation rate) were evaluated using the crosslinked sheets obtained in Examples 1C to 4C. The results are shown in Table 3.

[0191] <Crosslinking Properties> Using the resin compositions obtained in Examples 1C to 4C, a cure meter test was performed using a measuring device: MDR2000P (manufactured by ALPHA TECHNOLOGIES) under measurement conditions of 120°C and 30 minutes, and the torque increase (S'Max - S'Min) (dNm) was measured as follows. A sample was set in the measuring device, and the torque change obtained under constant temperature and constant shear rate conditions was measured to obtain a vulcanization curve. From this vulcanization curve, the minimum torque value S'Min (dNm) and the maximum torque value S'Max (dNm) were determined, and the progress of crosslinking was confirmed by the torque increase (S'Max - S'Min), and TC90 was determined. "TC90" is the time (in minutes (min)) it takes to reach a torque value that is the sum of the minimum torque value S'min and a torque value that is 90% of "S'max - S'min".

[0192] <Glass Adhesion> A transparent glass plate (AGC Fabricech, heat-treated float glass, 3 mm thick), the 0.5 mm thick uncrosslinked sheets obtained in Examples 1C to 4C, and a release PET sheet (Panac Co., Ltd., SP-PET-O1-50BU, 50 μm thick) were laminated together and placed in a vacuum laminator (NPC Co., Ltd., LM-50X50-S). The resulting laminate was placed on a hot plate heated to 120°C, and the pressure was reduced for 5 minutes and heated for 15 minutes to prepare a measurement sample consisting of a transparent glass plate / crosslinked sheet / release PET sheet laminate. The crosslinked sheet layer of this measurement sample was cut to a width of 10 mm, and the peel strength (glass adhesion strength) (N) with respect to glass was measured using a 180°C peel (tensile speed 300 mm / min, measurement temperature 23°C). For peel testing, a precision universal testing machine, Autograph (AGS-5KNG, manufactured by Shimadzu Corporation), was used. The average of three measurements was used as the glass adhesion (N).

[0193] <Gel Fraction> 100 mg of finely cut cross-linked sheets obtained in Examples 1C to 4C were wrapped in a 325-mesh screen and immersed in 30 ml of p-xylene in a sealed container at 140°C for 3 hours. Next, the screen was removed and vacuum-dried at 80°C for at least 2 hours until a constant weight was achieved. The gel fraction (mass%) was calculated using the following formula. The gel fraction is an indicator of the progress of cross-linking; a higher value means that cross-linking has progressed more. Gel Fraction (mass%) = 100 × (W ３ -W ２ ) / (W １ -W ２ ) (W １ : Mass of the screen and sample before testing, W ２ : Screen mass, W ３ (Mass of screen and sample after testing)

[0194] <Light Transmittance> For the crosslinked sheets obtained in Examples 1C to 4C, the light transmittance (%) was measured in the wavelength range of 200 to 1100 nm using a Hitachi High-Tech Science Co., Ltd. UV-Vis-Near-Infrared Spectrophotometer (UH4150). The average value of the light transmittance measured in the wavelength range of 380 to 1100 nm was defined as the light transmittance.

[0195] <Volume Resistivity> For the crosslinked sheets obtained in Examples 1C to 4C, the samples were left to stand for at least one hour under conditions of 23±2°C and 50±5% humidity. Then, in accordance with JIS K 6911:2006, 500V was applied for 300 seconds at 23°C, and the volume resistivity (Ω・cm) was measured. The average value over 200 to 300 seconds was used as the volume resistivity value. Volume resistivity was evaluated according to the following criteria: A: Volume resistivity of 1.0E+14Ω・cm or more B: Volume resistivity of less than 1.0E+14Ω・cm

[0196] <Creep (Elongation Deformation Rate)> The cross-linked sheets obtained in Examples 1C to 4C were cut into 10 mm x 70 mm strips, and markings were made 1 cm from both ends of the resulting strip-shaped samples to create measurement samples. Next, a double clip was attached to one end of the measurement sample and the sample was suspended from a stainless steel mesh rack. Then, a 10 g weight was attached to the other end of the measurement sample using the double clip, and the mesh rack was placed in an oven. The elongation deformation rate (%) of the sample was measured after 1 hour under conditions of 90°C.

[0197]

[0198] As shown in Table 3, the resin compositions of Examples 1C to 4C exhibit comparable light transmittance and volume resistivity, while also demonstrating superior crosslinking properties at low temperatures (e.g., 130°C or below).

Claims

1. Ethylene-α-olefin-non-conjugated polyene copolymer (A) having structural units derived from ethylene [A1], structural units derived from α-olefin [A2] having 4 or more carbon atoms, and structural units derived from non-conjugated polyene [A3] containing a total of two or more substructures selected from the group consisting of the following general formulas (I) and (II) in one molecule, and satisfying the following requirements (a1) to (a3): (a1) The content of structural units derived from ethylene [A1] is 75.0 to 95.0 mol%, with the total of structural units derived from [A1], [A2] and [A3] being 100 mol%; (a2) The content of structural units derived from α-olefin [A2] is 4.9 to 24.9 mol%, with the total of structural units derived from [A1], [A2] and [A3] being 100 mol%; (a3) The content of structural units derived from non-conjugated polyene [A3] is 0.1 to 1.0 mol%, with the total of structural units derived from [A1], [A2], and [A3] being 100 mol%.

2. The ethylene-α-olefin-non-conjugated polyene copolymer (A) according to claim 1, wherein the α-olefin [A2] having 4 or more carbon atoms is 1-butene.

3. The ethylene-α-olefin-nonconjugated polyene copolymer (A) according to claim 1, wherein the nonconjugated polyene [A3] contains 5-vinyl-2-norbornene.

4. The ethylene-α-olefin-non-conjugated polyene copolymer (A) according to claim 1, wherein the α-olefin [A2] having 4 or more carbon atoms is 1-butene, and the non-conjugated polyene [A3] contains 5-vinyl-2-norbornene.

5. The ethylene-α-olefin-non-conjugated polyene copolymer (A) according to claim 1, wherein the molar ratio [[A1] / [A3]] of structural units derived from ethylene [A1] to structural units derived from non-conjugated polyene [A3] is 100 to 1200.

6. The ethylene-α-olefin-non-conjugated polyene copolymer (A) according to claim 1, wherein the α-olefin [A2] having 4 or more carbon atoms is 1-butene, the non-conjugated polyene [A3] contains 5-vinyl-2-norbornene, and the molar ratio [[A1] / [A3]] of structural units derived from ethylene [A1] to structural units derived from non-conjugated polyene [A3] is 100 to 1200.

7. Furthermore, the ethylene-α-olefin-non-conjugated polyene copolymer (A) described in claim 1 satisfies the following requirement (a4): (a4) The melt flow rate measured at 190°C and a 2.16 kg load in accordance with ASTM D1238 is 3 to 20 g / 10 min.

8. Furthermore, the ethylene-α-olefin-non-conjugated polyene copolymer (A) according to claim 1, which satisfies the following requirement (a5): (a5) MFR １０ / MFR ２ However, it is in the range of 5.0 to 8.0 (MFR １０ This is the melt flow rate measured at 190°C and a 10 kg load in accordance with ASTM D1238, and MFR ２ This is the melt flow rate measured at 190°C and a 2.16 kg load, in accordance with ASTM D1238.

9. Furthermore, the ethylene-α-olefin-non-conjugated polyene copolymer (A) according to claim 1 satisfies the following requirement (a6): (a6) The glass transition temperature (Tg) measured by differential scanning calorimetry (DSC) is -50°C or lower.

10. The ethylene-α-olefin-non-conjugated polyene copolymer (A) according to claim 1, wherein the α-olefin [A2] having 4 or more carbon atoms is 1-butene, the non-conjugated polyene [A3] contains 5-vinyl-2-norbornene, the molar ratio [[A1] / [A3]] of structural units derived from ethylene [A1] to structural units derived from non-conjugated polyene [A3] is 100 to 1200, and the melt flow rate is 6.0 to 18 g / 10 min measured at 190°C and a 2.16 kg load in accordance with ASTM D1238.

11. A pellet comprising the ethylene-α-olefin-nonconjugated polyene copolymer (A) according to any one of claims 1 to 10.

12. A resin composition comprising the ethylene-α-olefin-nonconjugated polyene copolymer (A) described in claim 1, a hydrosilyl group-containing compound (D), and a platinum-based catalyst (E).

13. The resin composition according to claim 12, wherein the hydrosilyl group-containing compound (D) is an organohydrogenpolysiloxane represented by the following general formula (d). (In formula (d), n and p are each independently 0 or a positive integer, m is an integer of 1 to 20, and the sum of n, m and p is 5 to 50. A plurality of R １ and R ２ are each independently a monovalent alkyl group, R ａ is an aralkyl group, and the two R groups are each independently a hydrogen atom, R １ , R ２ , and R ａ a group selected from the group consisting of, and the group -[O-Si(R １ )(R ａ )]-, -[O-Si(R １ )H]- and -[O-Si(R １ )(R ２ )]- structural units may be arranged in blocks or may be arranged randomly. However, when n=1, at least one of the two R groups is a hydrogen atom, and when n=0, both of the two R groups are hydrogen atoms.) 14. The resin composition according to claim 12, comprising 0.1 to 100 parts by mass of the hydrosilyl group-containing compound (D) per 100 parts by mass of the ethylene-α-olefin-non-conjugated polyene copolymer (A), and comprising 0.000001 to 5 parts by mass of the platinum-based catalyst (E) per 100 parts by mass of the ethylene-α-olefin-non-conjugated polyene copolymer (A).

15. The resin composition according to claim 12, further comprising a reaction inhibitor (F), wherein the reaction inhibitor (F) is present in an amount of 0.001 to 5 parts by mass per 100 parts by mass of the ethylene-α-olefin-nonconjugated polyene copolymer (A).

16. The resin composition according to claim 12, further comprising an adhesion promoter (G) which is a silane-modified resin, wherein the adhesion promoter (G) is present in an amount of 10 to 40 parts by mass per 100 parts by mass of the ethylene-α-olefin-non-conjugated polyene copolymer (A).

17. An uncrosslinked sheet comprising the resin composition described in claim 12.

18. An uncrosslinked sheet according to claim 17, for use as a sealing material.

19. A crosslinked body obtained by crosslinking the resin composition described in claim 12 or the uncrosslinked sheet described in claim 17.

20. A sealing material comprising the crosslinked body described in claim 19.

21. The sealing material according to claim 20, for use with solar cells.

22. A solar cell module comprising a transparent protective member on the front side, a protective member on the back side, a solar cell element, and a sealing layer containing the sealing material described in claim 20, wherein the sealing layer seals the solar cell element between the transparent protective member on the front side and the protective member on the back side.

23. The solar cell module according to claim 22, wherein the solar cell element comprises at least one type of perovskite compound.

24. A method for manufacturing a solar cell module, comprising the steps of: (i) stacking a transparent protective member on the front side, an uncrosslinked sheet as described in claim 17, a solar cell element, and a protective member on the back side in this order to form a laminate; and (ii) pressing and heating the laminate to integrate it, wherein the heating temperature in step (ii) is 130°C or less.

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