JP2021054981A - Resin composition for sealing - Google Patents

Abstract

To provide a resin composition for sealing which is excellent in moisture permeability, and adhesion and transparency.SOLUTION: A resin composition for sealing contains (A) a polyolefin-based resin, (B) a moisture-absorbing filler, (C) a metal complex and (D) a tackifier. A content of the (B) moisture-absorbing filler to 100 mass% of a non-volatile component in the resin composition for sealing is more than 45 mass%, and the (C) metal complex is a metal complex in which a bidentate ligand having two ligand atoms that are oxygen atoms and a unidentate ligand having a ligand atom that is an oxygen atom are coupled to center metal.SELECTED DRAWING: None

Description

The present invention relates to a sealing resin composition, and more particularly to a sealing resin composition suitable for sealing an electronic device such as an organic EL (Electroluminescence) device or a solar cell.

A method of sealing an electronic device using a resin composition containing a hygroscopic filler in order to protect an electronic device, particularly an organic EL (Electroluminescence) device, a solar cell, or other moisture-sensitive electronic device from the outside air containing moisture or the like. Is known (Patent Document 1).

International Publication 2017/057708 Pamphlet

From the viewpoint of obtaining a sealing resin composition having high moisture permeability, it is desirable to increase the content of the hygroscopic filler in the resin composition, but if the content of the hygroscopic filler is increased, the resin composition There is a problem that the adhesiveness and transparency of the plastic are reduced. Therefore, an object of the present invention is to provide a sealing resin composition having excellent moisture permeation resistance and also excellent adhesiveness and transparency.

As a result of diligent studies to solve the above problems, the present inventors have blended a tackifier and a specific metal complex in a resin composition containing a polyolefin resin even when a hygroscopic filler is blended in a high content. In this case, they have found that the resin composition can be excellent in adhesiveness and transparency in addition to moisture permeation resistance, and have completed the present invention.

That is, the present invention has the following features.
[1] (A) Polyolefin-based resin;
(B) Hygroscopic filler;
A sealing resin composition containing (C) a metal complex; and (D) a tackifier, wherein the content of (B) a hygroscopic filler is 45 with respect to 100% by mass of a non-volatile component in the sealing resin composition. The metal complex (C) is a metal complex in which a bidentate ligand whose two coordinating atoms are both oxygen atoms and a monodentate ligand whose coordinating atom is an oxygen atom are bonded to the central metal. A resin composition for sealing.
[2] The sealing resin composition according to [1], wherein the hygroscopic filler is semi-calcined hydrotalcite.
[3] The sealing resin composition according to [1] or [2], wherein the central metal of the (C) metal complex is aluminum or titanium.
[4] The metal complex (C) has the general formula (1):

(During the ceremony,
M represents the metal of the 2nd to 6th periods of the periodic table,
R ₁ and R ₃ are independently hydrogen atoms, alkyl groups which may have substituents, alkoxy groups which may have substituents, aryl groups which may have substituents, or Represents an aralkyl group that may have a substituent,
R ₂ has a hydrogen atom, an alkyl group which may have a substituent, an alkoxy group which may have a substituent, an alkoxycarbonyl group which may have a substituent, and a substituent. Represents a good aryl group, or an alkoxy group which may have a substituent,
X represents a monodentate ligand whose coordination atom is an oxygen atom.
The solid line between the oxygen atom (O) and M in [] represents a covalent bond.
The dashed line between the oxygen atom (O) and M in [] represents the coordination bond, and m is an integer of 3 or 4, n is an integer of 1-3, and m> n. .. )
The sealing resin composition according to any one of [1] to [4], which is a metal complex represented by.
[5] The sealing resin composition according to [4], wherein M in the formula (1) is aluminum or titanium.
[6] The item according to any one of [1] to [5], wherein the (A) polyolefin-based resin contains a polyolefin-based resin having an acid anhydride group and / or a polyolefin-based resin having an epoxy group. Resin composition for sealing.
[7] The sealing resin according to any one of [1] to [5], wherein the (A) polyolefin-based resin contains a polyolefin-based resin having an acid anhydride group and a polyolefin-based resin having an epoxy group. Composition.
[8] The seal according to any one of [1] to [5], wherein the (A) polyolefin-based resin contains a reactant of a polyolefin-based resin having an acid anhydride group and a polyolefin-based resin having an epoxy group. Resin composition for stopping.
[9] The sealing according to any one of [1] to [8], wherein the content of the metal complex (C) is 0.1 to 5% by mass with respect to 100% by mass of the non-volatile component in the resin composition. Resin composition for.
[10] The sealing according to any one of [1] to [9], wherein the content of the tackifier (D) is 5 to 40% by mass with respect to 100% by mass of the non-volatile component in the resin composition. Resin composition.
[11] The sealing resin composition according to any one of [1] to [10], which is used for sealing an electronic device.
[12] The sealing resin composition according to [11], wherein the electronic device is an organic EL device or a solar cell.
[13] A sealing sheet containing a support and a layer of the resin composition according to any one of [1] to [12] formed on the support.
[14] An electronic device sealed with the sealing resin composition according to any one of [1] to [10].
[15] The electronic device according to [14], wherein the electronic device is an organic EL device or a solar cell.

According to the present invention, it is possible to realize a sealing resin composition having excellent adhesiveness and transparency in addition to moisture permeation resistance.

[Plastic composition for sealing]
The sealing resin composition of the present invention (hereinafter, also simply abbreviated as "resin composition") contains (A) polyolefin resin, (B) hygroscopic filler, (C) metal complex, and (C) metal complex as essential components. (D) Contains a tackifier.

<(A) Polyolefin resin>
The sealing resin composition of the present invention contains a polyolefin-based resin (hereinafter, also referred to as “component (A)”). The polyolefin-based resin can be used without particular limitation as long as it has an olefin-derived skeleton. The olefin is preferably a monoolefin having one olefinic carbon-carbon double bond and / or a diolefin having two olefinic carbon-carbon double bonds. Preferred examples of the monoolefin include α-olefins such as ethylene, propylene, 1-butene, isobutylene (isobutylene), 1-pentene, 1-hexene, 1-heptene and 1-octene, and examples of the diolefin include α-olefins. Preferably, 1,3-butadiene, isoprene, 1,3-pentadiene, 2,3-dimethylbutadiene and the like can be mentioned. The monoolefin and the diolefin may be one kind or two or more kinds each. Only one type of such polyolefin resin may be used, or two or more types may be used in combination.

The polyolefin-based resin may be a homopolymer, a random copolymer, or a block copolymer. Further, the copolymer is (i) a copolymer of two or more kinds of monoolefins, (ii) a copolymer of a monoolefin and a diolefin, or (iii) a monoolefin and an unsaturated carboxylic acid ester (for example, Examples thereof include copolymers with ethylenically unsaturated compounds (excluding diene-based monomers) other than olefins such as methyl methacrylate) and aromatic vinyl (for example, styrene).

The polyolefin-based resin is preferably a polybutene-based resin or a polypropylene-based resin. Here, the "polybutene-based resin" refers to a resin in which the main unit (maximum content unit) of all olefin monomer units constituting the polymer is derived from butene, and the "polypropylene-based resin" constitutes a polymer. Refers to a resin whose main unit (maximum content unit) is derived from propylene.

When the polybutene resin is a copolymer, examples of the monomer other than butene include styrene, ethylene, propylene, and isoprene. When the polypropylene-based resin is a copolymer, examples of the monomer other than propylene include ethylene, butene, and isoprene.

The polyolefin-based resin is a polyolefin-based resin having an acid anhydride group (that is, a carbonyloxycarbonyl group (-CO-O-CO-)) from the viewpoint of further improving the moisture permeability of the sealing resin composition. And / or a polyolefin resin having an epoxy group can be included. Examples of the acid anhydride group include a group derived from succinic anhydride, a group derived from maleic anhydride, a group derived from glutaric anhydride and the like. The acid anhydride group can have one kind or two or more kinds. The polyolefin-based resin having an acid anhydride group is, for example, an unsaturated compound having an acid anhydride group, and is obtained by graft-modifying the polyolefin resin under radical reaction conditions. Further, an unsaturated compound having an acid anhydride group may be radically copolymerized with an olefin. Similarly, the polyolefin-based resin having an epoxy group is an unsaturated compound having an epoxy group such as glycidyl (meth) acrylate, 4-hydroxybutyl acrylate glycidyl ether, and allyl glycidyl ether, and the polyolefin-based resin is subjected to radical reaction conditions. It is obtained by graft modification with. Further, the unsaturated compound having an epoxy group may be radically copolymerized together with the olefin.

As the polyolefin-based resin having an acid anhydride group, a polybutene-based resin having an acid anhydride group and a polypropylene-based resin having an acid anhydride group are preferable. Further, as the polyolefin-based resin having an epoxy group, a polybutene-based resin having an epoxy group and a polypropylene-based resin having an epoxy group are preferable.

In the polyolefin-based resin having an acid anhydride group, the concentration of the acid anhydride group in the resin is preferably 0.05 to 10 mmol / g, more preferably 0.1 to 5 mmol / g. The concentration of the acid anhydride group is obtained from the value of the acid value defined as the number of mg of potassium hydroxide required to neutralize the acid present in 1 g of the resin according to the description of JIS K 2501.

In the polyolefin-based resin having an epoxy group, the concentration of the epoxy group in the resin is preferably 0.05 to 10 mmol / g, more preferably 0.1 to 5 mmol / g. The epoxy group concentration is determined from the epoxy equivalent obtained based on JIS K 7236-1995.

The component (A) is an embodiment in which the polyolefin resin contains a polyolefin resin having an acid anhydride group and a polyolefin resin having an epoxy group from the viewpoint of further improving the moisture permeation resistance of the sealing resin composition. It is preferable to have.

Such a component (A) can form a crosslinked structure by reacting an acid anhydride group and an epoxy group by heating. When the component (A) contains a reactant of a polyolefin-based resin having an acid anhydride group and a polyolefin-based resin having an epoxy group as described above, the resin composition of the present invention is sealed with further improved moisture permeability and the like. Can form layers. The crosslinked structure can be formed after sealing with the resin composition (that is, after forming the sealing layer), but the device to be sealed includes an element that is sensitive to heat, such as an organic EL device. In this case, for example, it is desirable to form a crosslinked structure on the resin composition layer formed on the base material at the time of manufacturing the sealing sheet.

When the component (A) contains a polyolefin resin having an acid anhydride group and a polyolefin resin having an epoxy group, the reaction between the polyolefin resin having an epoxy group and the polyolefin resin having an acid anhydride group The amount ratio is not particularly limited as long as an appropriate crosslinked structure can be formed, but is a molar ratio of an epoxy group to an acid anhydride group (epoxide group: acid anhydride group), preferably 100: 10 to 100: 400, more preferably. Is 100: 25 to 100: 350, particularly preferably 100: 40 to 100: 300.

The number average molecular weight of the component (A) is not particularly limited, but the good coatability of the varnish when the sealing resin composition is processed into a film and the good phase with other components in the resin composition. From the viewpoint of providing solubility, 1,000,000 or less is preferable, 750,000 or less is more preferable, 500,000 or less is further preferable, and 400,000 or less is further preferable. On the other hand, from the viewpoint of preventing repelling during coating of the varnish of the sealing resin composition and improving the moisture permeability and mechanical strength of the forming sealing resin composition layer, 2,000 or more is preferable. 10,000 or more is more preferable, 30,000 or more is even more preferable, and 50,000 or more is particularly preferable. The number average molecular weight is measured by a gel permeation chromatography (GPC) method (polystyrene conversion). For the number average molecular weight by the GPC method, use LC-9A / RID-6A manufactured by Shimadzu Corporation as a measuring device, Shodex K-800P / K-804L / K-804L manufactured by Showa Denko Co., Ltd. as a column, and toluene or the like as a mobile phase. It can be measured at a column temperature of 40 ° C. and calculated using a standard polystyrene calibration curve.

Hereinafter, specific examples of the component (A) will be described.
As a specific example of the polypropylene-based resin, for example, "T-YP341" manufactured by Seikou PMC (glycidyl methacrylate-modified propylene-butene random copolymer, amount of butene unit per 100% by mass of propylene unit and butene unit in total: 29 mass). %, Epoxy group concentration: 0.638 mmol / g, Number average molecular weight: 155,000), "T-YP279" manufactured by Seikou PMC (maleic anhydride-modified propylene-butene random copolymer, total of propylene units and butene units Amount of butene unit per 100% by mass: 36% by mass, acid anhydride group concentration: 0.464 mmol / g, number average molecular weight: 35,000), Seikou PMC "T-YP276" (glycidyl methacrylate-modified propylene- Butene random copolymer, amount of butene unit per 100% by mass of propylene unit and butene unit: 36% by mass, epoxy group concentration: 0.638 mmol / g, number average molecular weight: 57,000), manufactured by Seikou PMC "T-YP312" (maleic anhydride-modified propylene-butene random copolymer, amount of butene units per 100% by mass of propylene units and butene units in total: 29% by mass, acid anhydride group concentration: 0.464 mmol / g, number average molecular weight: 60,900), "T-YP313" manufactured by Seikou PMC (glycidyl methacrylate-modified propylene-butene random copolymer, amount of butene units per 100% by mass of propylene units and butene units in total: 29) Mass%, epoxy group concentration: 0.638 mmol / g, number average molecular weight: 155,000) and the like.

Specific examples of the polybutene resin include, for example, HV-1900 (manufactured by JX Energy Co., Ltd.): polybutene (number average molecular weight: 2,900), HV-300M (manufactured by Toho Chemical Industry Co., Ltd.): maleic anhydride-modified liquid polybutene (manufactured by maleic anhydride). Acid anhydride group concentration: 0.77 mmol / g, number average molecular weight: 2,100), BASF's "Opanol B100" (polyisobutylene, viscosity average molecular weight: 1,110,000), BASF's "N50SF" ( Polyisobutylene, viscosity average molecular weight: 400,000) and the like can be mentioned.

The content of the component (A) in the sealing resin composition of the present invention is not particularly limited, but from the viewpoint of adhesiveness as the sealing resin composition, shape retention of the sealing layer, etc., and film processing. From the viewpoint of coatability and handleability (tack suppression) at the time, the content is preferably 50% by mass or less, more preferably 45% by mass or less, and more preferably 35% by mass, based on 100% by mass of the non-volatile component in the resin composition. More preferably, it is by mass or less. The content is preferably 10% by mass or more, more preferably 15% by mass or more, still more preferably 20% by mass or more, based on 100% by mass of the non-volatile component in the resin composition.

When the component (A) contains a polyolefin resin having an acid anhydride group and / or a polyolefin resin having an epoxy group, the polyolefin resin having an acid anhydride group per component (A) and / or the polyolefin resin having an acid anhydride group as a whole. / Or The amount of the polyolefin-based resin having an epoxy group is preferably 5 to 90% by mass, more preferably 10 to 80% by mass, and further preferably 15 to 70% by mass.

<(B) Hygroscopic filler>
The sealing resin composition of the present invention contains a hygroscopic filler (hereinafter, also referred to as “component (B)”).

The hygroscopic filler (B) is not particularly limited as long as it is a filler having an ability to absorb water, but metal oxides, metal hydroxides and the like are preferable. Specifically, metal oxides such as calcium oxide, magnesium oxide, strontium oxide, aluminum oxide, barium oxide, calcined hydrotalcite, calcined dolomite, calcium hydroxide, magnesium hydroxide, strontium hydroxide, aluminum hydroxide, and water. Examples thereof include metal hydroxides such as barium oxide and semi-baked hydrotalcite. Among them, semi-firing hydrotalcite and calcined hydrotalcite are preferable from the viewpoint of hygroscopicity, and semi-firing hydrotalcite is preferable from the viewpoint of transparency.

Hereinafter, calcined hydrotalcite and semi-firing hydrotalcite, which are preferable as hygroscopic fillers, will be described. Hydrotalcite can be classified into unfired hydrotalcite, semi-fired hydrotalcite, and fired hydrotalcite, and semi-fired hydrotalcite is particularly preferable from the viewpoint of transparency and moisture permeability of the resin composition. .. Unfired hydrotalcite is, for example, a metal hydroxide having a layered crystal structure typified by natural hydrotalcite _{(Mg 6 Al 2 (OH)} 16 CO 3 · 4H 2 O), for example, It consists of a basic skeleton layer [Mg _1-X Al _X (OH) ₂ ] ^{X +} and an intermediate layer [(CO ₃ ) _{X / 2} · mH ₂ O] ^X− . The uncalcined hydrotalcite in the present invention is a concept including hydrotalcite-like compounds such as synthetic hydrotalcite. Examples of the hydrotalcite-like compound include those represented by the following formulas (I) and (II).

^{_{[M 2+ 1-x M 3+}} x (OH) 2] x + · [(A n-) x / n · mH 2 O] x- (I)
^{(Wherein, M 2+} is ^Mg 2+, a divalent metal ion such as ^{Zn 2+, M 3+} represents a trivalent metal ion such as ^{Al 3+, Fe} 3+, ^{A n-} is _CO ³ 2-, Cl ^-, NO ₃ ^- represents a n-valent anion, such as a 0 <x <1, a 0 ≦ m <1, n is a positive number).
Wherein ^{(I), M 2+} is preferably ^{Mg 2+, M 3+} is preferably ^{Al 3+, A n-is} preferably _CO ^{3 2-.}

^{_{M 2+ x Al 2 (OH)}} 2x + 6-nz (A n-) z · mH 2 O (II)
^{(Wherein, M 2+} is ^Mg 2+, a divalent metal ion such as ^{Zn 2+, A n-} is ^{_{CO 3 2-, Cl -, NO}} 3 - represents a n-valent anion, such as, x is 2 or more Is a positive number, z is a positive number less than or equal to 2, m is a positive number, and n is a positive number.)
Wherein ^{(II), M 2+} is preferably ^{Mg 2+, A n-is} preferably _CO ^{3 2-.}

Semi-calcined hydrotalcite refers to a metal hydroxide having a layered crystal structure in which the amount of interlayer water is reduced or eliminated, which is obtained by calcining uncalcined hydrotalcite. The term "interlayer water" refers to _{"H 2} O" described in the above-mentioned composition formulas of uncalcined natural hydrotalcite and hydrotalcite-like compounds, if it is described using a composition formula.

On the other hand, calcined hydrotalcite refers to a metal oxide having an amorphous structure obtained by calcining uncalcined hydrotalcite or semi-calcined hydrotalcite, in which not only interlayer water but also hydroxyl groups are eliminated by condensation dehydration.

Uncalcined hydrotalcite, semi-calcined hydrotalcite and calcined hydrotalcite can be distinguished by the saturated water absorption rate. The saturated water absorption rate of the semi-baked hydrotalcite is 1% by weight or more and less than 20% by weight. On the other hand, the saturated water absorption rate of uncalcined hydrotalcite is less than 1% by weight, and the saturated water absorption rate of calcined hydrotalcite is 20% by weight or more.

The above "saturated water absorption rate" is determined by weighing 1.5 g of unfired hydrotalcite, semi-fired hydrotalcite, or fired hydrotalcite with a balance, measuring the initial mass, and then measuring the initial mass at 60 ° C., 90. The mass increase rate with respect to the initial mass when the product is allowed to stand in a small environmental tester (SH-222 manufactured by Espec Co., Ltd.) set to% RH (relative humidity) for 200 hours.
Saturated water absorption rate (mass%) = 100 × (mass after moisture absorption-initial mass) / initial mass (i)
Can be obtained at.

The saturated water absorption of the semi-baked hydrotalcite is preferably 3% by mass or more and less than 20% by mass, and more preferably 5% by mass or more and less than 20% by mass.

Further, uncalcined hydrotalcite, semi-calcined hydrotalcite and calcined hydrotalcite can be distinguished by the thermogravimetric reduction rate measured by thermogravimetric analysis. The thermogravimetric reduction rate of the semi-baked hydrotalcite at 280 ° C. is less than 15% by mass, and the thermogravimetric reduction rate at 380 ° C. is 12% by mass or more. On the other hand, the thermogravimetric reduction rate of uncalcined hydrotalcite at 280 ° C. is 15% by mass or more, and the thermogravimetric reduction rate of calcined hydrotalcite at 380 ° C. is less than 12% by mass.

For thermogravimetric analysis, 5 mg of hydrotalcite was weighed in an aluminum sample pan using TG / DTA EXSTAR6300 manufactured by Hitachi High-Tech Science Co., Ltd., and the nitrogen flow rate was 200 mL / min in an open state without a lid. It can be carried out from 30 ° C. to 550 ° C. under the condition of a heating rate of 10 ° C./min. The thermogravimetric reduction rate is calculated by the following formula (ii):
Thermogravimetric reduction rate (mass%)
= 100 × (mass before heating-mass when a predetermined temperature is reached) / mass before heating (ii)
Can be obtained at.

Further, uncalcined hydrotalcite, semi-calcined hydrotalcite and calcined hydrotalcite can be distinguished by the peak and the relative intensity ratio measured by powder X-ray diffraction. Semi-baked hydrotalcite shows a peak in which 2θ is split into two in the vicinity of 8 to 18 ° by powder X-ray diffraction, or a peak with a shoulder due to the combination of the two peaks, and the peak or shoulder that appears on the low angle side The relative intensity ratio (low-angle side diffraction intensity / high-angle side diffraction intensity) of the diffraction intensity (= low-angle side diffraction intensity) and the diffraction intensity of the peak or shoulder appearing on the high-angle side (= high-angle side diffraction intensity) is 0.001. ~ 1,000. On the other hand, uncalcined hydrotalcite has only one peak near 8 to 18 °, or the relative intensity ratio of the diffraction intensity of the peak or shoulder appearing on the low angle side and the peak or shoulder appearing on the high angle side is in the above range. Be outside. The calcined hydrotalcite does not have a characteristic peak in the region of 8 ° to 18 °, but has a characteristic peak in the region of 43 °. Powder X-ray diffraction measurement is performed by a powder X-ray diffractometer (PANalytical, Empyrena) with anti-cathode CuKα (1.5405 Å), voltage: 45 V, current: 40 mA, sampling width: 0.0260 °, scanning speed: 0. The measurement was performed under the conditions of .0657 ° / s and the measurement diffraction angle range (2θ): 5.0131 to 79.9711 °. The peak search uses the peak search function of the software attached to the diffractometer, and "minimum significance: 0.50, minimum peak tip: 0.01 °, maximum peak tip: 1.00 °, peak base width: 2". It can be performed under the condition of "0.00 °, method: minimum value of second derivative".

Specific examples of uncalcined hydrotalcite, semi-calcined hydrotalcite and calcined hydrotalcite include the following.
-DHT-4C (manufactured by Kyowa Chemical Industry Co., Ltd.): Semi-fired hydrotalcite (average particle size: 400 nm, BET specific surface area: 15 m ² / g)
-DHT-4A-2 (manufactured by Kyowa Chemical Industry Co., Ltd.): Semi-calcined hydrotalcite (average particle size: 400 nm, BET specific surface area: 13 m ² / g)
-KW-2200 (manufactured by Kyowa Chemical Industry Co., Ltd.): calcined hydrotalcite (average particle size: 400 nm, BET specific surface area: 146 m ² / g)
-DHT-4A (manufactured by Kyowa Chemical Industry Co., Ltd.): Unfired hydrotalcite (average particle size: 400 nm, BET specific surface area: 10 m ² / g)

The average particle size of the hygroscopic filler is not particularly limited, but is preferably 25 μm or less, more preferably 15 μm or less, still more preferably 10 μm or less, from the viewpoint of the influence on the object to be sealed and the moisture permeation resistance. 5 μm or less is particularly preferable, and 1 μm or less is most preferable. On the other hand, from the viewpoint of the dispersibility of the hygroscopic filler and the viscosity of the resin composition, the average particle size is preferably 0.001 μm or more, more preferably 0.01 μm or more, still more preferably 0.1 μm or more.

The average particle size of the hygroscopic filler can be measured by a laser diffraction / scattering method based on the Mie scattering theory. Specifically, it can be measured by creating a particle size distribution of the hygroscopic filler on a volume basis with a laser diffraction type particle size distribution measuring device and using the median diameter as the average particle size. As the measurement sample, a hygroscopic filler dispersed in water by ultrasonic waves can be preferably used. As the laser diffraction type particle size distribution measuring device, LA-500 manufactured by HORIBA, Ltd. or the like can be used.

Of the hygroscopic fillers, the average particle size of hydrotalcite is preferably 1 to 1,000 nm, more preferably 10 to 800 nm. The average particle size of hydrotalcite is the median size of the particle size distribution when the particle size distribution is prepared on a volume basis by laser diffraction scattering type particle size distribution measurement (JIS Z 8825).

Of the hygroscopic filler, BET specific surface area of the hydrotalcite is preferably ^{1~250m 2 / g, 5~200m 2 /} g is more preferable. The BET specific surface area of hydrotalcite can be calculated by adsorbing nitrogen gas on the sample surface using a specific surface area measuring device (Macsorb HM Model 1210 Mountec) according to the BET method and using the BET multipoint method. ..

As the component (B), one that has been surface-treated with a surface treatment agent can be used. As the surface treatment agent used for the surface treatment, for example, higher fatty acids, alkylsilanes, silane coupling agents and the like can be used, and among them, higher fatty acids and alkylsilanes are preferable. As the surface treatment agent, one kind or two or more kinds can be used.

Examples of the higher fatty acid include higher fatty acids having 18 or more carbon atoms such as stearic acid, montanic acid, myristic acid, and palmitic acid, and stearic acid is preferable. These may be used alone or in combination of two or more. Examples of alkylsilanes include methyltrimethoxysilane, ethyltrimethoxysilane, hexyltrimethoxysilane, octyltrimethoxysilane, decyltrimethoxysilane, octadecyltrimethoxysilane, dimethyldimethoxysilane, octyltriethoxysilane, and n-octadecyldimethyl (n-octadecyldimethyl). Examples thereof include 3- (trimethoxysilyl) propyl) ammonium chloride. These may be used alone or in combination of two or more. Examples of the silane coupling agent include 3-glycidyloxypropyltrimethoxysilane, 3-glycidyloxypropyltriethoxysilane, 3-glycidyloxypropyl (dimethoxy) methylsilane and 2- (3,4-epoxycyclohexyl) ethyltrimethoxy. Epoxy-based silane coupling agents such as silane; mercapto-based silane coupling agents such as 3-mercaptopropyltrimethoxysilane, 3-mercaptopropyltriethoxysilane, 3-mercaptopropylmethyldimethoxysilane and 11-mercaptoundecyltrimethoxysilane 3-Aminopropyltrimethoxysilane, 3-aminopropyltriethoxysilane, 3-aminopropyldimethoxymethylsilane, N-phenyl-3-aminopropyltrimethoxysilane, N-methylaminopropyltrimethoxysilane, N- (2) Amino-based silane coupling agents such as −aminoethyl) -3-aminopropyltrimethoxysilane and N- (2-aminoethyl) -3-aminopropyldimethoxymethylsilane; Coupling agents, vinyl-based silane coupling agents such as vinyltrimethoxysilane, vinyltriethoxysilane and vinylmethyldiethoxysilane; styryl-based silane coupling agents such as p-styryltrimethoxysilane; 3-acrylicoxypropyltrimethoxy Acrylic silane coupling agents such as silane and 3-methacryloxypropyltrimethoxysilane; isocyanate-based silane coupling agents such as 3-isocyanvopropyltrimethoxysilane, bis (triethoxysilylpropyl) disulfide, bis (triethoxysilylpropyl) ) A sulfide-based silane coupling agent such as tetrasulfide; phenyltrimethoxysilane, methacryloxypropyltrimethoxysilane, imidazolesilane, triazinesilane and the like can be mentioned. These may be used alone or in combination of two or more.

The surface treatment of the component (B) can be carried out, for example, by stirring the untreated component (B) at room temperature with a mixer, adding and spraying a surface treatment agent, and stirring for 5 to 60 minutes. As the mixer, a known mixer can be used, and examples thereof include blenders such as V blenders, ribbon blenders and bubble cone blenders, mixers such as Henshell mixers and concrete mixers, ball mills and cutter mills. Further, when pulverizing the moisture absorbing material with a ball mill or the like, a method of mixing the above-mentioned higher fatty acid, alkylsilanes or silane coupling agent and surface-treating the material is also possible. The treatment amount of the surface treatment agent varies depending on the type of the component (B), the type of the surface treatment agent, and the like, but is preferably 1 to 10 parts by mass with respect to 100 parts by mass of the component (B).

The content of the component (B) in the resin composition is more than 45% by mass with respect to 100% by mass of the non-volatile component in the resin composition from the viewpoint of moisture permeation resistance. The content is preferably 46% by mass or more, more preferably 48% by mass or more, and further preferably 50% by mass or more. The upper limit of the content is not particularly limited as long as the effect of the present invention is exhibited, but from the viewpoint of adhesiveness and transparency of the resin composition, it is preferable with respect to 100% by mass of the non-volatile component in the resin composition. It is 80% by mass or less, more preferably 75% by mass or less, and further preferably 70% by mass or less.

<(C) Metal complex>
The resin composition of the present invention contains a metal complex (hereinafter, also referred to as “component (C)”). As the metal complex (C) in the present invention, a metal complex in which a bidentate ligand in which two coordinating atoms are both oxygen atoms and a monodentate ligand in which the coordinating atom is an oxygen atom is bonded to the central metal is used. To do.

In the present invention, a metal complex is a chemical species in which another atom, molecule, or ion is bonded to a metal atom or an ion. The ligand refers to a molecule or ion bonded to a metal atom or ion. Further, an atom directly involved in the bond is called a coordinating atom, a ligand having two coordinating atoms is called a bidentate ligand, and a ligand having one coordinating atom is called a monodentate ligand.

The component (C) consists of a bidentate ligand in which both of the two coordinating atoms are oxygen atoms (hereinafter, also abbreviated as "oxygen / bidentate ligand") and a monodentate coordination in which the coordinating atom is an oxygen atom. Any metal complex having a structure in which the child (hereinafter, also abbreviated as “oxygen / monodentate ligand”) is bonded to the central metal is not particularly limited, and a known metal complex satisfying the structure can be used. .. Among them, a metal complex in which the central metal is a metal in the second to sixth periods of the periodic table is preferable, a metal complex in which the central metal is a metal in the third to fifth periods is more preferable, and a metal complex in which the central metal is a metal in the third to fifth periods is more preferable. A metal complex in which the metal is Al, Ti, Mn, Fe, Co, Ni, Cu, Zn, Ge, Zr, In, or Sn, and more preferably a metal complex in which the central metal is Al, Ti, or Zr. is there. From the viewpoint of transparency of the resin composition, a metal complex in which the central metal is Al (aluminum) or Ti (titanium) is particularly preferable. As the component (C), one kind or two or more kinds can be used.

Examples of the oxygen / bidentate ligand include a compound represented by the following formula (a).

In formula (a), R ₁ , R ₂ , and R ₃ are synonymous with those in formula (1) below.

The compound represented by the formula (a) represents an oxygen / bidentate ligand before coordination with the central metal. In the present invention, the oxygen / bidentate ligand in the state of being coordinated to the central metal and the oxygen / bidentate ligand before being coordinated to the central metal are not particularly distinguished as “oxygen / bidentate”. Sometimes referred to as a "coordinated ligand". The specific example of the compound represented by the formula (a) is synonymous with the specific example of the oxygen / bidentate ligand in the metal complex represented by the formula (1) described later.

Examples of the oxygen / monodentate ligand include an alkoxide anion (RO ⁻ ) and a carboxylate anion (RCOO ⁻ ). Specific examples of the oxygen / monodentate ligand are also synonymous with specific examples of the oxygen / monodentate ligand in the metal complex represented by the following formula (1). In the present invention, the oxygen / monodentate ligand coordinated to the central metal and the oxygen / monodentate ligand (alcohol (ROH), carboxylic acid (RCOOH)) before coordination to the central metal are particularly used. Without distinction, it may be referred to as "oxygen / monodentate ligand".

Further, in the metal complex of the component (C), the number of oxygen / bidentate ligands is 1 or more, preferably 1 or more and 3 or less, and more preferably 2. When the number of oxygen / bidentate ligands is plural, they may be the same ligand or different ligands, but the same ligand is preferable. The number of oxygen / monodentate ligands is 1 or more, preferably 1 or more and 3 or less, and more preferably 2 or 3. When there are a plurality of oxygen / monodentate ligands, they may be the same ligand or different ligands, but the same ligand is preferable.

As the component (C), a metal complex represented by the following general formula (1) (hereinafter, also referred to as a metal complex of the formula (1)) is more preferable.

In equation (1)
M is the central metal of the metal complex and represents the metal of the 2nd to 6th periods of the periodic table. It is preferably a metal having a third to fifth period, more preferably Al, Ti, Mn, Fe, Co, Ni, Cu, Zn, Ge, Zr, In, or Sn, and even more preferably Al, Ti. , Or Zr, and particularly preferably Al (aluminum) or Ti (titanium).
R ₁ and R ₃ independently represent a hydrogen atom, an alkyl group, an alkoxy group, an aryl group, or an aralkyl group, respectively.
R ₂ represents a hydrogen atom, an alkyl group, an alkoxy group, an alkoxycarbonyl group, an aryl group, or an aralkyl group.
X represents an oxygen / monodentate ligand.

The solid line between the oxygen atom (O) and M in [] represents a covalent bond, and the broken line between the oxygen atom (O) and M in [] represents a coordination bond.

m is an integer of 3 or 4, n is an integer of 1-3, and m> n.

The alkyl groups at R ₁ , R ₂ , and R ₃ may be linear or branched. The alkyl group preferably has 1 to 20 carbon atoms, more preferably 1 to 10 carbon atoms, and particularly preferably 1 to 6 carbon atoms. Examples of the alkyl group include a methyl group, an ethyl group, a propyl group, an isopropyl group, a butyl group, an isobutyl group, a sec-butyl group, a tert-butyl group, a pentyl group, an isopentyl group, a neopentyl group, and a 1-ethylpropyl group. Examples thereof include hexyl group, isohexyl group, 1,1-dimethylbutyl group, 2,2-dimethylbutyl group, 3,3-dimethylbutyl group and 2-ethylbutyl group. The alkyl group may have a substituent. Examples of the substituent include a halogen atom, a hydroxy group, an amino group which may have a substituent, and the like.

Examples of the halogen atom include a fluorine atom, a chlorine atom, a bromine atom, and an iodine atom. Examples of the amino group which may have the above-mentioned substituent include an amino group, a mono- or di-alkylamino group (eg, a methylamino group, a dimethylamino group, an ethylamino group, a diethylamino group and a propylamino group). , Dibutylamino group), mono- or di-cycloalkylamino group (eg, cyclopropylamino group, cyclohexylamino group), mono- or di-arylamino group (eg, phenylamino group), mono- or di-aralkyl Examples thereof include an amino group (eg, benzylamino group, dibenzylamino group), a heterocyclic amino group (eg, pyridylamino group) and the like.

The alkoxy group in R ₁ , R ₂ , and R ₃ is preferably an alkoxy group having 1 to 6 carbon atoms, for example, a methoxy group, an ethoxy group, a propoxy group, an isopropoxy group, a butoxy group, an isobutoxy group, sec. -Butoxy group, tert-butoxy group, pentyloxy group, hexyloxy group and the like can be mentioned. The alkoxy group may have a substituent. Examples of the substituent include a halogen atom, a hydroxy group, an amino group which may have a substituent, and the like. Specific examples of the halogen atom and the specific example of the amino group which may have a substituent are the same as described above.

The aryl group in R ₁ , R ₂ , and R ₃ has preferably 6 to 18 carbon atoms, more preferably 6 to 14 carbon atoms. Examples of the aryl group include a phenyl group, a 1-naphthyl group, a 2-naphthyl group, a 1-anthryl group, a 2-anthryl group, a 9-anthryl group and the like. The aryl group may have a substituent. Examples of the substituent include a halogen atom, a hydroxy group, an alkyl group which may have a substituent, an alkenyl group which may have a substituent, and an alkynyl group which may have a substituent. Examples thereof include an amino group which may have a substituent.

The above alkenyl group may be linear or branched. The alkenyl group preferably has 2 to 10 carbon atoms, more preferably 2 to 6 carbon atoms. For example, an ethenyl group (ie, vinyl group), 1-propenyl group, 2-propenyl group, 2-methyl-1-propenyl group, 1-butenyl group, 2-butenyl group, 3-butenyl group, 3-methyl-2. -Butenyl group, 1-pentenyl group, 2-pentenyl group, 3-pentenyl group, 4-pentenyl group, 4-methyl-3-pentenyl group, 1-hexenyl group, 3-hexenyl group, 5-hexenyl group and the like. Be done. Examples of the substituent which the alkenyl group may have include a halogen atom, a hydroxy group, an amino group which may have a substituent and the like. Specific examples of the halogen atom and the specific example of the amino group which may have a substituent are the same as described above.

The alkynyl group described above may be either linear or branched. The alkynyl group preferably has 2 to 10 carbon atoms, more preferably 2 to 6 carbon atoms. For example, ethynyl group, 1-propynyl group, 2-propynyl group, 1-butynyl group, 2-butynyl group, 3-butynyl group, 1-pentynyl group, 2-pentynyl group, 3-pentynyl group, 4-pentynyl group, Examples thereof include 1-hexynyl group, 2-hexynyl group, 3-hexynyl group, 4-hexynyl group, 5-hexynyl group, 4-methyl-2-pentynyl group and the like. Examples of the substituent that the alkynyl group may have include a halogen atom, a hydroxy group, an amino group that may have a substituent, and the like. Specific examples of the halogen atom and the specific example of the amino group which may have a substituent are the same as described above.

The carbon number of the aralkyl group in R ₁ , R ₂ , and R _{3 is preferably 7 to 16.} For example, a benzyl group, a phenethyl group, a naphthylmethyl group, a phenylpropyl group and the like can be mentioned. The aralkyl group may have a substituent. Examples of the substituent include a halogen atom, a hydroxy group, an amino group which may have a substituent, and the like. Specific examples of the halogen atom and the specific example of the amino group which may have a substituent are the same as described above.

Alkoxycarbonyl group in R ₂ is preferably an alkoxycarbonyl group having carbon atoms in the alkoxy is 1 to 6, for example, methoxycarbonyl group, ethoxycarbonyl group, propoxycarbonyl group, isopropoxycarbonyl group, butoxycarbonyl group, isobutoxy Examples thereof include a carbonyl group, a sec-butoxycarbonyl group, a tert-butoxycarbonyl group, a pentyloxycarbonyl group, a hexyloxycarbonyl group and the like. The alkoxycarbonyl group may have a substituent. Examples of the substituent include a halogen atom, a hydroxy group, an amino group which may have a substituent, and the like. Specific examples of the halogen atom are the same as those of the halogen atom which is the substituent of the above-mentioned alkyl group, and specific examples of the amino group which may have a substituent are the above-mentioned substitution which is the substituent of the alkyl group. Similar to that of an amino group which may have a group.

In the formula, the oxygen / monodentate ligand represented by X is usually a conjugate base of Bronsted acid, and examples thereof include an alkoxide anion (RO ⁻ ) and a carboxylate anion (RCOO ⁻ ).

In the alkoxide anion (RO ⁻ ), the organic group R may be either an aliphatic group or an aromatic group. Further, the aliphatic group may be either a saturated aliphatic group or an unsaturated aliphatic group. The organic group R preferably has 1 to 20 carbon atoms, more preferably 1 to 10 carbon atoms, and particularly preferably 1 to 6 carbon atoms. Examples of the alkoxide anion (RO ⁻ ) include methoxide, ethoxide, propoxide, isopropoxide, butoxide, isobutoxide, sec-butoxide, tert-butoxide, pentyl oxide, hexyl oxide and the like.

In the carboxylate anion (RCOO ⁻ ), the organic group R may be either an aliphatic group or an aromatic group. Further, the aliphatic group may be either a saturated aliphatic group or an unsaturated aliphatic group. The organic group R preferably has 1 to 20 carbon atoms, more preferably 1 to 10 carbon atoms, and particularly preferably 1 to 6 carbon atoms. Examples of the carboxylate anion (RCOO ⁻ ) include a carboxylate anion corresponding to a carboxylic acid such as acetic acid, propionic acid, and benzoic acid.

The inside of [] in the formula represents the oxygen / bidentate ligand. Specific examples of oxygen / bidentate ligands include acetylacetone, 3-methyl-2,4-pentandione, acetylacetoacetic acid, 2,4-hexanedione, 2,4-heptandione, 5-methyl-2,4. -Hexanedione, 5,5-dimethyl-2,4-hexanedione, benzoylacetone, benzoylacetophenone, salicylaldehyde, 1,1,1-trifluoroacetylacetone, 1,1,1,5,5,5-hexafluoro Acetylacetone, 3-methoxy-2,4-pentandione, 3-cyano-2,4-pentandione, 3-nitro-2,4-pentandione, 3-chloro-2,4-pentandione, acetoacetic acid, aceto Examples thereof include methyl acetate, ethyl acetoacetone, propyl acetoacetate, salicylic acid, methyl salicylate, malonic acid, dimethyl malonate, diethyl malonate and the like. In the state of coordination to the central metal, the oxygen / bidentate ligand has a structure in which one or more protons are removed from it.

Specific examples of the metal complex of the formula (1) include the following. As a metal complex in which the central metal M is Al (aluminum), for example, aluminum alkyl acetoacetate diisopropylate (aluminum 9-octadecynyl aceto-acetate diisopropoxide), aluminum ethyl acetoacetate diisopropylate, aluminum ethyl acetoacetate Examples thereof include din-butylate, aluminum propyl acetoacetate diisopropylate, and aluminum n-butyl acetoacetate diisopropylate.

Further, as a metal complex in which the central metal M is Ti (titanium), for example, titanium allylacetacetate triisopropoxyside, titaniumdi-n-butoxide (bis-2,4-pentandionate), titanium diisopropoxyside bis (titanium diisopropoxyside bis). Tetramethylheptandionate), titanium diisopropoxyside bis (ethylacetacetate), titanium methylphenoxide, titanium oxide bis (pentandionate) and the like.

Further, as a metal complex in which the central metal M is Zr (zirconium), for example, zirconium allylacetoacetate triisopropoxide, zirconium di-n-butoxide (bis-2,4-pentandionate), zirconium diisopropoxide (zirconium diisopropoxide) Bis-2,4-pentandionate), zirconium diisopropoxide bis (tetramethylheptanionate), zirconium diisopropoxide bis (ethylacetate acetate), zirconium butoxide (acetylacetate) (bisethylacetacetate), Examples thereof include zirconium tributoxymonoacetylacetonate.

The content of the component (C) in the resin composition is not particularly limited, but from the viewpoint of adhesiveness and transparency of the resin composition, 0.1% by mass with respect to 100% by mass of the non-volatile component in the resin composition. The above is preferable, and 0.3% by mass or more is more preferable. Further, from the viewpoint of facilitating the influence of the outgas derived from the component (C) on the sealing target, the content thereof is preferably 5% by mass or less, preferably 3% by mass, based on 100% by mass of the non-volatile component in the resin composition. % Or less is more preferable.

In one embodiment of the present invention, the content of the component (C) in the resin composition of the present invention is preferably 0.1 to 5% by mass with respect to 100% by mass of the non-volatile component in the resin composition. Yes, more preferably 0.3 to 3% by mass.

Even if the metal complex is different from the component (C) of the present invention, for example, a metal complex in which an oxygen / bidentate ligand is bonded to the central metal, the oxygen / monodentate ligand is not bonded to the central metal. Even if it is a metal complex or a metal complex in which an oxygen / monodentate ligand is bonded to a central metal, or a metal complex in which an oxygen / bidentate ligand is not bonded to the central metal, the purpose is excellent. It is not possible to realize a resin composition having both adhesiveness, transparency and moisture permeation resistance. The reason is not always clear, but the metal complex having a structure in which the oxygen / bidentate ligand and the oxygen / monodentate ligand, which are the components (C) of the present invention, are bonded to the central metal, is an oxygen that is easily hydrolyzed. -Since it has a monodentate ligand, it is easy to modify the surface of the hygroscopic filler which is the component (B), the component (B) can be sufficiently dispersed in the resin composition, and the resin composition is sealed. When attached to the object to be stopped, the oxygen / bidentate ligand chelate-exchanges with the functional groups on the surface of the glass, plastic, inorganic film, etc. existing on the surface of the object to be sealed to form a strong bond (B). Even when the components are blended in a high content, it is presumed that the resin composition has excellent adhesiveness and transparency in addition to moisture permeation resistance.

<(D) Adhesive imparting agent>
The sealing resin composition of the present invention contains a tackifier (hereinafter, also abbreviated as "component (D)").

The tackifier is not particularly limited, and is terpen resin, terpenphenol resin, rosin resin, hydrogenated terpen resin, aromatic modified terpen resin, etc., kumaron resin, inden resin, petroleum resin (aliphatic petroleum). Resins, hydrogenated alicyclic petroleum resins, aromatic petroleum resins, aliphatic aromatic copolymerized petroleum resins, alicyclic petroleum resins, dicyclopentadiene (hereinafter, also abbreviated as "DCPD") petroleum resins, Hydrogenated dicyclopentadiene-based petroleum resin, etc.), etc., but from the viewpoint of adhesiveness and transparency, dicyclopentadiene-based petroleum resin and hydrogenated dicyclopentadiene-based petroleum resin are more preferable, and hydrogenated dicyclopentadiene-based petroleum resin is more preferable. Petroleum resin is particularly preferable.

The content of the component (D) in the resin composition is not particularly limited, but is preferably 5% by mass or more with respect to 100% by mass of the non-volatile component in the resin composition from the viewpoint of adhesiveness of the resin composition and the like. 10% by mass or more is more preferable, and 15% by mass or more is further preferable. Further, from the viewpoint of adhesive stability in a high temperature region, the content is preferably 40% by mass or less, more preferably 30% by mass or less, and more preferably 25% by mass or less, based on 100% by mass of the non-volatile component in the resin composition. More preferred.

In one embodiment of the present invention, the content of the component (D) in the resin composition of the present invention is preferably 5 to 40% by mass with respect to 100% by mass of the non-volatile component in the resin composition. It is more preferably 10 to 30% by mass, and even more preferably 15 to 25% by mass.

<(E) Additive>
To the extent that the effects of the present invention are not impaired, the resin composition of the present invention includes softeners such as mineral oil-based softeners, vegetable oil-based softeners, subfactis, fatty acids, fatty acid salts, synthetic organic compounds, and synthetic oils; Agents: Organic fillers such as rubber particles, silicone powders, nylon powders, fluororesin powders; silicone-based, fluorine-based, polymer-based defoaming agents or leveling agents; triazole compounds, thiazole compounds, triazine compounds, porphyrin compounds, etc. Adhesion-imparting agents; thickeners such as Orben and Benton; antioxidants; heat stabilizers; additives such as light stabilizers can be blended. Further, an inorganic filler other than the hygroscopic filler may be blended. Examples of such inorganic fillers include silica, mica, alumina, barium sulfate, talc, clay, mica powder, calcium carbonate, magnesium carbonate, boron nitride, aluminum borate, barium titanate, strontium titanate, and calcium titanate. , Magnesium titanate, bismuth titanate, titanium oxide, barium titanate, calcium titanate and the like.

<(F) Curing agent and / or curing accelerator>
The resin composition of the present invention may contain a curing agent and / or a curing accelerator, for example, when it contains a polyisobutylene-based resin having an epoxy group or the like. As the curing agent and / or the curing accelerator, only one type may be used, or two or more types may be used in combination. Examples of the curing agent include imidazole compounds, tertiary / quaternary amine compounds, dimethylurea compounds, organic phosphine compounds, primary / secondary amine compounds, and the like. Examples of the curing accelerator include imidazole compounds, tertiary and quaternary amine compounds, dimethylurea compounds, organic phosphine compounds and the like.

Examples of the imidazole compound as a curing agent and / or curing accelerator in the present invention include 1H-imidazole, 2-methylimidazole, 2-phenyl-4-methylimidazole, 2-ethyl-4-methylimidazole, and 1-cyanoethyl. -2-Ethyl-4-methylimidazole, 2-undecylimidazole, 1-cyanoethyl-2-undecylimidazole, 1-cyanoethyl-2-undecylimidazolium trimerite, 2,4-diamino-6- (2) '-Undecylimidazolyl- (1'))-ethyl-s-triazine, 2-phenyl-4,5-bis (hydroxymethyl) imidazole, 1-benzyl-2-methylimidazole, 1-benzyl-2-phenylimidazole , 2-Phenylimidazole, 2-dodecylimidazole, 2-heptadecylimidazole, 1,2-dimethylimidazole, 2-phenyl-4-methyl-5-hydroxymethylimidazole, 2,4-diamino-6- (2'-) Examples thereof include methylimidazolyl- (1') -ethyl-s-triazine, 2,4-diamino-6- (2'-methylimidazolyl- (1'))-ethyl-s-triazine isocyanuric acid adduct, and the like. Specific examples of the compound include Curesol 2MZ, 2P4MZ, 2E4MZ, 2E4MZ-CN, C11Z, C11Z-CN, C11Z-CNS, C11Z-A, 2PHZ, 1B2MZ, 1B2PZ, 2PZ, C17Z, 1.2DMZ, 2P4MHZ-PW, 2MZ-A, 2MA-OK (both manufactured by Shikoku Kasei Kogyo Co., Ltd.) and the like can be mentioned.

The tertiary / quaternary amine-based curing agent as the curing agent and / or the curing accelerator in the present invention is not particularly limited, but is a quaternary ammonium salt such as tetramethylammonium bromide or tetrabutylammonium bromide; DBU (1). , 8-diazabicyclo [5.4.0] undecene-7), DBN (1,5-diazabicyclo [4.3.0] nonen-5), DBU-phenol salt, DBU-octylate, DBU-p- Diazabicyclo compounds such as toluene sulfonate, DBU-gerate, DBU-phenol novolak resin salt; benzyl dimethylamine, 2- (dimethylaminomethyl) phenol, 2,4,6-tris (diaminomethyl) phenol (TAP), etc. Tertiary amines and salts thereof, dimethylurea compounds such as aromatic dimethylurea and aliphatic dimethylurea; and the like.

Examples of the primary and secondary amine compounds as the curing agent in the present invention include the aliphatic amines diethylenetriamine, triethylenetetraamine, tetraethylenepentamine, trimethylhexamethylenediamine, 2-methylpentamethylenediamine, and 1 , 3-Bisaminomethylcyclohexane, Dipropylenediamine, diethylaminopropylamine, Bis (4-aminocyclohexyl) methane, Norbornenediamine, 1,2-diaminocyclohexane, etc., N-aminoethylpyverazine, which is an alicyclic amine, Examples thereof include diaminodiphenylmethane, m-phenylenediamine, m-xylenediamine, metaphenylenediamine, diaminodiphenylmethane, diaminodiphenylsulfone, diethyltoluenediamine, which are aromatic amines such as 1,4-bis (3-aminopropyl) piperazine. .. Specific examples of the primary and secondary amine compounds include Kayahard A-A (manufactured by Nippon Kayaku Co., Ltd .: 4,4'-diamino-3,3'-dimethyldiphenylmethane).

Specific examples of the dimethylurea compound as a curing agent and / or curing accelerator in the present invention include DCMU (3- (3,4-dichlorophenyl) -1,1-dimethylurea) and U-CAT3512T (manufactured by San-Apro). Aromatic dimethylurea such as, and aliphatic dimethylurea such as U-CAT3503N (manufactured by San-Apro Co., Ltd.) can be mentioned. Among them, aromatic dimethylurea is preferably used from the viewpoint of curability.

Examples of the organophosphine compound as a curing agent and / or a curing accelerator in the present invention include triphenylphosphine, triphenylphosphinenium tetra-p-trilborate, tetraphenylphosphonium tetraphenylborate, and tri-tert-butylphosphonium tetraphenyl. Examples thereof include borate, (4-methylphenyl) triphenylphosphonium thiocyanate, tetraphenylphosphonium thiocyanate, butyltriphenylphosphonium thiocyanate, triphenylphosphine triphenylborane and the like. Specific examples of the organic phosphine compound include TPP, TPP-MK, TPP-K, TTBuP-K, TPP-SCN, TPP-S (manufactured by Hokuko Chemical Industry Co., Ltd.) and the like.

The content of the curing agent and / or the curing accelerator in the resin composition is not particularly limited, but from the viewpoint of preventing deterioration of the transparency of the sealing layer (resin composition layer), etc., in the resin composition. It is preferably 5% by mass or less, more preferably 1% by mass or less, based on 100% by mass of the non-volatile component. On the other hand, from the viewpoint of suppressing the tack of the sealing layer, the content is preferably 0.0005% by mass or more, more preferably 0.001% by mass or more, based on 100% by mass of the non-volatile component in the resin composition. ..

<(G) Organic solvent>
The resin composition of the present invention contains, for example, an organic solvent from the viewpoint of coatability of the resin composition when producing a sealing sheet in which a layer of the resin composition is formed on a support described later. Can be blended. Examples of the organic solvent include ketones such as acetone, methyl ethyl ketone (hereinafter, also abbreviated as “MEK”) and cyclohexanone, and acetic acid esters such as ethyl acetate, butyl acetate, cellosolve acetate, propylene glycol monomethyl ether acetate and carbitol acetate. , Carbitols such as cellosolve and butylcarbitol, aromatic hydrocarbons such as toluene and xylene, dimethylformamide, dimethylacetamide, N-methylpyrrolidone and the like. Only one kind of such organic solvent may be used, or two or more kinds may be used in combination. The amount of the organic solvent is not particularly limited, but from the viewpoint of coatability, it is preferable to use an amount having a viscosity (25 ° C.) of the resin composition of 300 to 2000 mPa · s.

<Manufacturing method of resin composition>
The resin composition of the present invention can be produced by mixing the above-mentioned components (including at least the components (A) to (D)) using a kneading roller, a rotary mixer, or the like.

<Sealing sheet>
For example, the present invention is applied onto a support by applying the resin composition of the present invention made into a varnish by blending an organic solvent onto the support and drying the obtained coating film by heating or blowing hot air. A sealing sheet, which is a sheet on which a layer of the resin composition of the above is formed, is obtained. In the case of a sealing sheet prepared by using a resin composition containing a polyolefin resin having an acid anhydride group and a polyolefin resin having an epoxy group as the component (A) in the resin composition, at the time of its preparation, By reacting the acid anhydride group and the epoxy group to form a crosslinked structure, the moisture permeation resistance of the layer of the resin composition is enhanced, and the sealing performance (the ability to block moisture and oxygen in the air, etc.) A higher sealing sheet is obtained.

Examples of the support used for the sealing sheet include polyolefins such as polyethylene, polypropylene and polyvinyl chloride, polyethylene terephthalate (hereinafter sometimes abbreviated as "PET"), polyesters such as polyethylene naphthalate, polycarbonate and polyimide. Plastic film can be mentioned. PET is particularly preferable as the plastic film. Further, the support may be a metal foil such as aluminum foil, stainless steel foil, or copper foil. The support may be subjected to a mold release treatment in addition to the mat treatment and the corona treatment (hereinafter, the “support after the mold release treatment” is also referred to as a “peelable support”). Examples of the mold release treatment include a mold release treatment using a mold release agent such as a silicone resin-based mold release agent, an alkyd resin-based mold release agent, and a fluororesin-based mold release agent. When the support has a release layer in the present invention, the release layer is also regarded as a part of the support. The thickness of the support is not particularly limited, but is preferably 20 to 200 μm, more preferably 20 to 125 μm from the viewpoint of handleability and the like.

The peelable support is a support in which one side of the resin composition of the present invention on which a layer is formed is subjected to a mold release treatment, and before the sealing sheet is actually used for forming the sealing structure. It is a support that is peeled off. For this reason, the peelable support does not necessarily have to be moisture-proof, but from the viewpoint of preventing moisture from entering the layer of the resin composition during the storage period until the sealing sheet is subjected to sealing. , It is preferable to have moisture resistance. In order to improve the moisture-proof property of the sealing sheet, a plastic film having a barrier layer may be used as a support (hereinafter, the plastic film having such a barrier layer is also referred to as a "moisture-proof support"). Examples of the barrier layer include nitrides such as silicon nitride, oxides such as aluminum oxide, stainless steel foil, and metal foil of aluminum foil. Examples of the plastic film include the above-mentioned plastic film. A commercially available product may be used as the plastic film having the barrier layer. Further, the moisture-proof support may be a film obtained by composite laminating a metal foil and a plastic film. For example, examples of commercially available polyethylene terephthalate films with aluminum foil include "PET Tsuki AL1N30" manufactured by Tokai Toyo Aluminum Sales Co., Ltd. and "PET Tsuki AL3025" manufactured by Fukuda Metal Co., Ltd. Further, one having a multi-layer structure of two or more layers, for example, one in which the above plastic film and the above metal foil are bonded together via an adhesive can also be used. This is inexpensive and is advantageous from the viewpoint of handleability.

In the sealing sheet, the layer of the resin composition may be protected by a protective film. By protecting with a protective film, it is possible to prevent dust and the like from adhering to the surface of the resin composition layer and scratches. As the protective film, it is preferable to use a plastic film similar to the support. Further, the protective film may also be subjected to a mold release treatment in addition to the matte treatment and the corona treatment. The thickness of the protective film is not particularly limited, but is usually 1 to 150 μm, preferably 10 to 100 μm.

If a support having moisture resistance and high transmittance is used for the sealing sheet, the sealing sheet is laminated on the sealing target to provide high moisture permeability. A sealed structure can be formed. Examples of such a support having moisture resistance and high transmittance include a plastic film on which an inorganic substance such as silicon oxide (silica), silicon nitride, SiCN, or amorphous silicon is vapor-deposited on the surface. Examples of the plastic film include polyolefins such as polyethylene, polypropylene and polyvinyl chloride, polyesters such as polyethylene terephthalate and polyethylene naphthalate, polycarbonate and polyimide. PET is particularly preferable as the plastic film. Examples of commercially available moisture-proof plastic films include Tech Barrier HX, AX, LX, L series (manufactured by Mitsubishi Plastics) and X-BARRIER (manufactured by Mitsubishi Plastics) with further enhanced moisture-proof effect. Be done. As the support, a support having a multi-layer structure of two or more layers may be used.

In the case of a sealing sheet having a peelable support, the sealing sheet is laminated on the sealing target, the support is peeled off, and a separately prepared sealing base material (a moisture-proof plastic film, (Metal foil such as copper foil and aluminum foil) can be laminated.

A circular polarizing plate can be used for the support of the sealing sheet of the present invention. Generally, a circular polarizing plate is composed of a polarizing plate and a quarter wave plate. When a circular polarizing plate is used as a support, a 1/4 wave plate is generally arranged on the resin composition layer side. When a support including both a circularly polarizing plate and a moisture-proof support is used, the moisture-proof support is preferably arranged on the resin composition layer side, and the 1/4 wavelength plate of the circularly polarizing plate is on the moisture-proof support side. Is placed in. The moisture-proof support and the circular polarizing plate can be adhered with an adhesive or the like, and the adhesive is not particularly limited as long as it is a highly transparent adhesive. For example, an acrylic adhesive or a polyvinyl alcohol adhesive. Etc. are used.

A protective film for protecting the polarizer (polarizing plate) can be provided on the circular polarizing plate, and a known protective film can also be used. For example, Japanese Patent Application Laid-Open No. 2016-105166 and International Publication No. 2016-105166 can be used. The protective film described in the publication 2014/003189 pamphlet and the like can be mentioned.

In the sealing sheet of the present invention, the support is preferably composed of at least one selected from a peelable support, a moisture-proof support, and a circular polarizing plate.

<Electronic device>
When sealing an electronic device with the resin composition of the present invention, it is preferable to use the sealing sheet for sealing. That is, by laminating the sealing sheet of the present invention on the electronic device portion provided with the sealing structure, the electronic device sealed with the sealing resin composition of the present invention can be obtained.

Since the sealing resin composition of the present invention has excellent moisture permeability, adhesiveness and transparency, it is used for electronic devices, particularly electronic devices such as organic EL devices and solar cells, which are required to have these characteristics. It can be suitably used as a sealing resin composition.

Hereinafter, the present invention will be described in more detail with reference to Examples, but the present invention is not limited to these Examples. In the following description, "parts" and "%" in the amounts of the component and the copolymerization unit mean "parts by mass" and "% by mass", respectively, unless otherwise specified.

The raw materials used in Examples and Comparative Examples are as follows.
(A) Polyolefin resin T-YP312 (manufactured by Seikou PMC): Maleic anhydride-modified propylene-butene copolymer (propylene unit / butene unit = 71% / 29%, acid anhydride group concentration: 0.464 mmol / 40% toluene solution of g, number average molecular weight: 60,900) ・ T-YP313 (manufactured by Seikou PMC): Glycidyl methacrylate-modified propylene-butene copolymer (propylene unit / butene unit = 71% / 29%, epoxy group 40% toluene solution with concentration: 0.638 mmol / g, number average molecular weight: 155,000) ・ T-YP341 (manufactured by Starlight PMC): Glycidyl methacrylate-modified propylene-butene random copolymer (propylene unit / butene unit: 71) 20% silicone solution of% / 29%, glycidyl group concentration: 0.638 mmol / g, number average molecular weight: 155,000) ・ HV-1900 (manufactured by JX Energy Co., Ltd.): Polybutene (number average molecular weight: 2,900)
HV-300M (manufactured by Toho Chemical Industry Co., Ltd.): Maleic anhydride-modified liquid polybutene (acid anhydride group concentration: 0.77 mmol / g, number average molecular weight: 2,100)

(B) Hygroscopic filler DHT-4C (manufactured by Kyowa Chemical Industry Co., Ltd.): Semi-fired hydrotalcite (abbreviated as "semi-fired HT" in Table 1) (Average particle size: 400 nm, BET specific surface area: 15 m ²⁾ / G)

(C) Metal Complex Aluminum Chelate M (manufactured by Kawaken Fine Chemicals): Aluminum Alkyl Acetacetate Diisopropylate KR38S (manufactured by Ajinomoto Fine Techno): Isopropyltris (Dioctylpyrophosphate) Titanate Organites ZC540 (Matsumoto Fine Chemicals) (Manufactured by Matsumoto Fine Chemical Co., Ltd.): Zirconium Tributoxymonoacetylacetone Organite Organix ZC320 (manufactured by Matsumoto Fine Chemical Co., Ltd.): Zirconium stearate

(D) Adhesive-imparting agent, Alcon P125 (manufactured by Arakawa Chemical Co., Ltd.): Cyclohexane ring-containing saturated hydrocarbon resin, softening point 125 ° C.
-T-REZ HA125 (manufactured by TonenGeneral): Hydrogenated DCPD type hydrocarbon resin (softening point 125 ° C)

(F) Curing agent / anionic polymerization type amine-based curing agent (2,4,6-tris (diaminomethyl) phenol, hereinafter abbreviated as "TAP")

(G) Organic solvent / toluene

Others ・ Swazole # 1000 (manufactured by Maruzen Petrochemical Co., Ltd.): Aromatic mixed solvent

The varnish of the resin composition was prepared by the following procedure at the compounding ratio shown in Table 1, and then a sealing sheet was prepared.
<Example 1>
77 parts of cyclohexane ring-containing saturated hydrocarbon resin (Arcon P125, 60% swazole solution), 35 parts of maleic anhydride-modified liquid polyisobutylene (HV-300M), 60 parts of polybutene (HV-1900), aluminum alkylacetate diisopropi 1.5 parts of rate (aluminum chelate M) and 270 parts of semi-baked hydrotalcite (DHT-4C) were dispersed in 3 rolls to obtain a mixture. To the obtained mixture, 40 parts of a glycidyl methacrylate-modified polypropylene-polybutene copolymer (T-YP341, 20% silicone solution), 0.5 part of an anionic polymerization amine-based curing agent (TAP) and 170 parts of toluene were added. The obtained mixture was uniformly dispersed with a high-speed rotary mixer to obtain a varnish of a resin composition. The varnish is uniformly applied to the release-treated surface of a polyethylene terephthalate film (thickness 38 μm) (hereinafter referred to as PET film) treated with a silicone-based mold release agent with a die coater, and heated at 140 ° C. for 30 minutes. A resin composition layer having a thickness of 20 μm (residual solvent amount in the resin composition layer: about 1% by mass) was formed, and then a cover film (PET film treated with a silicone-based release agent (thickness 38 μm)). Was bonded to obtain a sealing sheet.

<Example 2>
Sealed in the same manner as in Example 1 except that 1.5 parts of zirconium tributoxymonoacetylacetone (Organix ZC540) was used instead of 1.5 parts of aluminum alkylacetate diisopropyrate (aluminum chelate M). I got a stop sheet.

<Example 3>
Instead of 77 parts of a cyclohexane ring-containing saturated hydrocarbon resin (Arcon P125, 60% silicone solution), 77 parts of a hydrogenated DCPD type hydrocarbon resin (T-REZ HA125) was used, and aluminum alkylacetate diisopropyrate (aluminum chelate M) was used. ) Was added in 1 part, and the semi-baked hydrotalcite (DHT-4C) was added in 200 parts in the same manner as in Example 1 to obtain a sealing sheet.

<Example 4>
For sealing in the same manner as in Example 1 except that polybutene (HV-1900) was not added and the amount of cyclohexane ring-containing saturated hydrocarbon resin (Arcon P125, 60% silicone solution) was 137 parts. I got a sheet.

<Example 5>
Same as in Example 1 except that the amount of aluminum alkylacetate diisopropirate (aluminum chelate M) added was 1.8 parts and the amount of semi-calcined hydrotalcite (DHT-4C) was 350 parts. A sheet for sealing was obtained.

<Example 6>
77 parts of cyclohexane ring-containing saturated hydrocarbon resin (Arcon P125, 60% silicone solution), 95 parts of polybutene (HV-1900), 1 part of aluminum alkylacetate diisopropyrate (aluminum chelate M), and semi-baked hydrotalcite. 200 parts (DHT-4C) were dispersed in 3 rolls to obtain a mixture. To the obtained mixture, 20 parts of a glycidyl methacrylate-modified polypropylene-polybutene copolymer (T-YP312, 40% toluene solution) and 20 parts of a maleic anhydride-modified propylene-butene copolymer (T-YP313, 40% toluene solution). , 0.5 part of anionic polymerization type amine-based curing agent (TAP) and 170 parts of toluene were blended, and the obtained mixture was uniformly dispersed with a high-speed rotary mixer to obtain a varnish of a resin composition. Using the obtained varnish, a sealing sheet was obtained in the same manner as in Example 1.

<Comparative example 1>
A sealing sheet was prepared in the same manner as in Example 3 except that 1 part of isopropyltris (dioctylpyrophosphate) titanate (KR38S) was used instead of 1 part of aluminum alkylacetate acetate diisopropylate (aluminum chelate M). Obtained.

<Comparative example 2>
A sealing sheet was prepared in the same manner as in Example 1 except that 1.5 parts of zirconium stearate (Organix ZC320) was used instead of 1.5 parts of aluminum alkylacetate acetate diisopropylate (aluminum chelate M). Obtained.

<Comparative example 3>
A sealing sheet was obtained in the same manner as in Example 1 except that aluminum alkyl acetoacetate diisopropylate (aluminum chelate M) was not added.

<Comparative example 4>
For sealing in the same manner as in Example 6 except that aluminum alkyl acetoacetate diisopropylate (aluminum chelate M) was not added and the amount of semi-baked hydrotalcite (DHT-4C) added was 100 parts. I got a sheet.

<Measurement method / evaluation method>
Various measurement methods and evaluation methods will be described below.

<Evaluation of adhesiveness>
The cover film of the sealing sheet (cut to a length of 50 mm and a width of 20 mm) produced in Examples and Comparative Examples was peeled off, and the resin composition layer was separated into a batch type vacuum laminator (manufactured by Nichigo Morton, V-160). ) Was laminated on an aluminum foil / PET composite film "PET Tsuki AL1N30" (aluminum foil: 30 μm, PET: 25 μm: trade name manufactured by Toyo Aluminum Sales Co., Ltd.) having a length of 100 mm and a width of 25 mm. Lamination was performed under the conditions of a temperature of 80 ° C., a time of 300 seconds, and a pressure of 0.3 MPa. Then, the PET film was peeled off, and a glass plate (length 76 mm, width 26 mm, thickness 1.2 mm, microslide glass) was further laminated on the exposed resin composition layer under the same conditions as described above. The adhesiveness of the obtained laminate was measured by the peel strength when peeled at a tensile speed of 300 mm / min in the 180 degree direction with respect to the length direction of the aluminum foil / PET composite film.
Good (○): Peel strength is 0.2 kgf / cm or more Poor (×): Peel strength is less than 0.2 kgf / cm

<Evaluation of transparency>
The sealing sheets produced in Examples and Comparative Examples were cut into a length of 50 mm and a width of 20 mm, the cover film was peeled off, and then the resin composition layer was formed into a glass plate (length 76 mm, width 26 mm and thickness 1.2 mm). Microslide glass; White slide glass S1112 manufactured by Matsunami Glass Industry Co., Ltd. No. 2) was laminated with a batch type vacuum laminator (Nichigo Morton Co., Ltd., V-160) to obtain a sample for evaluation. The laminating conditions were a temperature of 80 ° C., a reduced pressure time of 30 seconds, and then a pressure of 0.3 MPa for 30 seconds. Peel off the PET film of the sealing sheet, measure the haze of the evaluation sample (thickness 20 μm) with D65 light using air as a reference using a haze meter manufactured by Suga Test Instruments Co., Ltd., and determine the transparency according to the following criteria. evaluated.
Good (○): Haze less than 3.5% Bad (×): Haze 3.5% or more

<Evaluation of moisture permeability>
In each example and comparative example, instead of the PET film (support) treated with the silicone-based mold release agent, the aluminum foil / PET composite film "PET Tsuki AL1N30" (aluminum foil: 30 μm, PET: 25 μm, Tokai Toyo A sealing sheet was obtained in the same manner as in each Example and Comparative Example except that the product name of the aluminum distributor) was used.

The moisture permeation resistance of each sealing sheet was evaluated by using non-alkali glass vapor-deposited with calcium as a model of the issuing surface of the organic EL device and measuring the emission area reduction start time of the organic EL device (calcium (calcium (calcium)). Ca) test). A 50 mm × 50 mm square of non-alkali glass was washed with boiling isopropeel alcohol for 5 minutes and dried at 150 ° C. for 30 minutes or more. Calcium (purity 99.8%) was vapor-deposited (thickness 300 nm) using the glass and a mask having a distance of 3 mm from the end. A sealing sheet having the same resin composition layer as in each Example and Comparative Example was heated in a glove box at 130 ° C. for 1 hour, and then calcium-deposited non-alkali glass was placed in a glove box with a thermal laminator (manufactured by Fujipla). A laminated body (evaluation sample) was prepared by laminating with each sealing sheet with Lamipacker DAiSY A4 (LPD2325).

When calcium comes into contact with water and becomes calcium oxide, it changes from white to transparent. Therefore, the intrusion of water into the evaluation sample can be evaluated by measuring the distance (mm) from the edge of the evaluation sample to the white calcium. Therefore, an evaluation sample containing calcium was used as a model of the light emitting surface of the organic EL device.

First, the distance of the deposited calcium from the end of the evaluation sample was measured by a Measuring Microscope MF-U manufactured by Mitutoyo Co., Ltd., and this value was used as an initial value. Next, the evaluation sample was allowed to stand for a certain period of time in a small environmental tester (SH-222 manufactured by Espec) set at a temperature of 85 ° C. and 85% RH, and at regular time intervals, from the end of the evaluation sample to calcium. Distance was measured. The following Fick diffusion formula:

(In the formula, X indicates the distance (mm) from the end of the evaluation sample to calcium, t indicates the time (hr) that the evaluation sample was allowed to stand in a small environmental tester, and K indicates the proportionality constant. Show.)
Based on, the proportionality constant K is calculated by drawing a theoretical curve by the least squares method from the "distance from the edge of the evaluation sample to calcium" and the "time when the evaluation sample is allowed to stand in a small environmental tester". did. Using the calculated K, the time at which X = 2.6 mm was calculated as the emission area reduction start time. The higher the moisture permeation resistance, the slower the rate of moisture intrusion, and the longer the emission area reduction start time.
Good (○): 250 hr or more Bad (×): Less than 250 hr

From the results in Table 1, it was shown that the sealing sheets of Examples 1 to 6 were excellent not only in moisture permeation resistance but also in adhesiveness and transparency. On the other hand, the sealing sheets of Comparative Examples 1 and 3 are excellent in adhesiveness but inferior in transparency, and the sealing sheets of Comparative Example 2 are excellent in moisture permeability and transparency, but have excellent adhesiveness. It turns out to be low. Further, it can be seen that the sealing sheet of Comparative Example 4 is excellent in adhesiveness and transparency, but inferior in moisture permeation resistance.

Since the sealing resin composition of the present invention is excellent in adhesiveness and transparency in addition to moisture permeation resistance, it is suitably used for sealing electronic devices, particularly electronic devices such as organic EL devices and solar cells. Can be done.

Claims (15)

(A) Polyolefin-based resin;
(B) Hygroscopic filler;
A sealing resin composition containing (C) a metal complex; and (D) a tackifier, wherein the content of (B) a hygroscopic filler is 45 with respect to 100% by mass of a non-volatile component in the sealing resin composition. The metal complex (C) is a metal complex in which a bidentate ligand whose two coordinating atoms are both oxygen atoms and a monodentate ligand whose coordinating atom is an oxygen atom are bonded to the central metal. A resin composition for sealing. (B) The sealing resin composition according to claim 1, wherein the hygroscopic filler is semi-baked hydrotalcite. (C) The sealing resin composition according to claim 1 or 2, wherein the central metal of the metal complex is aluminum or titanium. The metal complex (C) has the general formula (1):

(During the ceremony,
M represents the metal of the 2nd to 6th periods of the periodic table,
R ₁ and R ₃ are independently hydrogen atoms, alkyl groups which may have substituents, alkoxy groups which may have substituents, aryl groups which may have substituents, or Represents an aralkyl group that may have a substituent,
R ₂ has a hydrogen atom, an alkyl group which may have a substituent, an alkoxy group which may have a substituent, an alkoxycarbonyl group which may have a substituent, and a substituent. Represents a good aryl group, or an alkoxy group which may have a substituent,
X represents a monodentate ligand whose coordination atom is an oxygen atom.
The solid line between the oxygen atom (O) and M in [] represents a covalent bond.
The dashed line between the oxygen atom (O) and M in [] represents the coordination bond, and m is an integer of 3 or 4, n is an integer of 1-3, and m> n. .. )
The sealing resin composition according to any one of claims 1 to 4, which is a metal complex represented by. The sealing resin composition according to claim 4, wherein M in the formula (1) is aluminum or titanium. The sealing resin composition according to any one of claims 1 to 5, wherein the polyolefin-based resin (A) contains a polyolefin-based resin having an acid anhydride group and / or a polyolefin-based resin having an epoxy group. Stuff. The sealing resin composition according to any one of claims 1 to 5, wherein the polyolefin-based resin (A) contains a polyolefin-based resin having an acid anhydride group and a polyolefin-based resin having an epoxy group. The sealing resin composition according to any one of claims 1 to 5, wherein the polyolefin-based resin (A) contains a reactant of a polyolefin-based resin having an acid anhydride group and a polyolefin-based resin having an epoxy group. .. The sealing resin composition according to any one of claims 1 to 8, wherein the content of the metal complex (C) is 0.1 to 5% by mass with respect to 100% by mass of the non-volatile component in the resin composition. The sealing resin composition according to any one of claims 1 to 9, wherein the content of the tackifier (D) is 5 to 40% by mass with respect to 100% by mass of the non-volatile component in the resin composition. The sealing resin composition according to any one of claims 1 to 10, which is used for sealing an electronic device. The sealing resin composition according to claim 11, wherein the electronic device is an organic EL device or a solar cell. A sealing sheet comprising a support and a layer of the resin composition according to any one of claims 1 to 12 formed on the support. An electronic device sealed with the sealing resin composition according to any one of claims 1 to 10. The electronic device according to claim 14, wherein the electronic device is an organic EL device or a solar cell.