JPH06336506A - Highly dielectric ultraviolet-curable composition and its use - Google Patents

Abstract

PURPOSE:To obtain the subject composition useful as a binder for the reflective insulation layer and the luminescent layer of an electroluminescent element of organic dispersion type, for forming a dielectric film for a film capacitor, and as a matrix resin for an ionically conductive polymeric material. CONSTITUTION:This composition comprises a cyanoethylated monomer represented by the formula (wherein (m) is 1-3; 1<=m<=(n-1); R<1> is H of CH3; and R<2> is a linear or branched alkylene optionally having at least one of oxygen, phenylene, hydrogenated phenylene, and amino) and an ultraviolet polymerization initiator.

Description

Detailed Description of the Invention

[0001]

FIELD OF THE INVENTION The present invention relates to a UV-curable high dielectric composition and its use, and more specifically, it comprises a specific cyanoethylated monomer which is photocurable in a liquid state at room temperature and an UV polymerization initiator. As a binder for each of the reflective insulating layer and the light emitting layer in an organic dispersion type electroluminescence (EL) element, or for forming a dielectric film of a film capacitor, a film battery, an electrochromic element (ECD), an organic electrolyte capacitor, an electrocardiogram or The present invention relates to an ultraviolet curable high dielectric composition useful as a matrix resin of a polymer ion conductive material used for an electrode (conductor) for a human body of medical equipment for low to high frequency treatment.

[0002]

2. Description of the Related Art An organic dispersion type EL device is generally constructed by laminating a back electrode, a reflective insulating layer, a light emitting layer and a transparent electrode in this order. Among them, as a binder for each of the reflective insulating layer and the light emitting layer, a high dielectric resin (for example, a cyanoethylated product of a fibrin-based polymer such as cellulose, polyvinyl alcohol, or phenoxy resin or a polymer having a large number of hydroxyl groups) was dissolved in an organic solvent. A resin solution is used. By the way, in such an organic dispersion type EL device, inorganic high dielectric material powder is mixed in the resin solution in the reflective insulating layer and phosphor powder is mixed in the light emitting layer, and the mixture thereof is applied by screen printing or a bar coater. It is manufactured by heating and drying to remove the organic solvent, forming a reflective insulating layer and a light emitting layer respectively, and then thermocompression bonding (lamination).

However, in such production, organic solvents such as N, N-dimethylformamide, N, N are used.
-Dimethylacetamide, dimethyl sulfoxide, N-
Solvents such as methyl-2-pyrrolidone and γ-butyrolactone are used, but these solvents are used only as a role of a viscosity reducing agent for coating, and therefore, in the organic dispersion type EL device. If it remains, it will show only adverse effects such as a decrease in life and efficiency, and it will be harmful to the human body, and will eventually cause global environmental pollution, recovery and drying equipment of organic solvents and its cost,
There is energy loss and the like, and solvent-free methods are strongly demanded from these problems.

Film capacitors generally include polyester (PET), polypropylene, polystyrene,
Resin films such as polycarbonate, polyvinylidene fluoride, and polyphenyl sulfone are used as the dielectric, but an electrode is required, and usually, a metal film such as aluminum is vapor-deposited (metallized) on this dielectric film,
A stack of a dielectric film and a metal foil such as aluminum is used. However, there is a strong demand for miniaturization of film capacitors, and various studies have been made.
Such miniaturization is to increase the dielectric constant of the dielectric material and to reduce the thickness of the dielectric film as much as possible.

On the other hand, a so-called polymer solid electrolyte in which an electrolyte salt such as an alkali metal salt is dissolved in a matrix resin having a main structure of polyoxyethylene has been studied as the above-mentioned polymer ion conductive material. However, there are many problems in electrical conductivity, especially in low temperature electrical conductivity and mechanical strength. Further, the polymer-based ionic conductive material has the above-mentioned applications, but in particular, as a solid electrolyte for light, thin, short, and small batteries represented by a film battery, among them, particularly as a solid electrolyte of a lithium secondary battery, a large ionic conductivity, It is required that the decrease is small even at low temperatures, and that mechanical bending resistance and strength are large, but there is still not enough.

[0006]

Then, the inventors of the present invention firstly conducted diligent studies to solve the problems of the organic dispersion type EL device, and as a result, instead of the conventional binder resin solution, the liquid crystal at room temperature was used. Using a specific curable cyanoethylated monomer and UV-curable composition of UV-polymerization initiator, it can be easily mixed and dispersed with inorganic high-dielectric material powder and phosphor powder without solvent, and can be applied at high pressure. It was found that it is extremely useful for the intended purpose as a binder because it rapidly cures (polymerizes) when irradiated with ultraviolet light from a mercury lamp or the like.

The above-mentioned ultraviolet-curable composition has a high dielectric constant, and is directly applied thinly on a metal foil and cured by irradiation with ultraviolet rays to form a thin film having a high dielectric constant (film). I knew that it was possible. There is a limit to the thinness of the dielectric film in conventional film capacitors in terms of handling in the manufacturing process (strength, wrinkles, wrinkles, etc.),
Even if handled accurately, the limit is about 10 μ, but if it is applied on a metal foil, it is possible to greatly reduce the thickness. It should be noted that the thinning of the dielectric film causes a decrease in withstand voltage, but the circuit voltage of most recent electronic circuits is low and there is no problem.

Further, when the above ultraviolet curable composition is used as a matrix resin of a polymeric ion conductive material,
It was found that UV irradiation can provide a solid electrolyte having good performance requirements such as ionic conductivity and mechanical strength at low temperatures.

That is, the present invention has the formula:

[Chemical 2] (In the formula, 1 ≦ m ≦ n−1, m is 1 to 3, R ¹ is H or CH ₃ , and R ² has at least one of an oxygen atom, a phenylene group, a hydrogenated phenylene group and an amino group. A cyanoethylated monomer [I] represented by a certain linear or branched alkylene group); and a UV polymerization initiator, and a back electrode, An organic dispersion-type EL device comprising a reflective insulating layer, a light emitting layer, and a transparent electrode, which are laminated in this order, using the ultraviolet curable high dielectric composition as a binder for the reflective insulating layer and the light emitting layer. And (i) after applying the dispersion of the ultraviolet curable high dielectric composition and the inorganic high dielectric material powder to the back electrode and irradiating with ultraviolet rays to form a reflective insulating layer. , The dispersion of the ultraviolet curable high dielectric composition and the phosphor powder on the reflective insulating layer is overlapped and irradiated with ultraviolet rays to form a light emitting layer, and then transparent electrodes are overlapped and thermocompression bonded, or (Ii) The back electrode is coated with the dispersion of the ultraviolet-curable high-dielectric composition and the inorganic high-dielectric material powder and irradiated with ultraviolet rays to form a reflective insulating layer, and then the ultraviolet-curable high-resistant layer is formed on the reflective insulating layer. The dielectric composition and the phosphor powder dispersion are applied over each other, a transparent electrode is overlaid thereon, and pressure-bonded at room temperature, and ultraviolet irradiation is performed from above the transparent electrode, or (i
ii) A back electrode is coated with a dispersion of the above-mentioned UV-curable high dielectric composition and inorganic high-dielectric material powder and irradiated with UV rays to form a reflective insulating layer, while, on the other hand, a transparent electrode is subjected to the above-mentioned UV-curable high dielectric composition. Characterized by applying a dispersion of the phosphor and phosphor powder, irradiating ultraviolet rays to form a light emitting layer, and then thermocompression-bonding both electrodes so that the reflective insulating layer of the back electrode and the light emitting layer of the transparent electrode face each other. The present invention provides a polymer-based ion conductive material characterized by using the above-mentioned ultraviolet-curable high dielectric composition as a matrix resin and a method for producing an organic dispersion-type EL device.

The cyanoethylated monomer [I] used in the present invention can be produced according to the following procedure. That is, first, the formula:

[Chemical 3] 1 mol of the n-valent polyhydroxyl compound [II] of 1 mol of acrylonitrile is subjected to a Michael addition reaction in the presence of an acid or alkali catalyst at 20 to 100 ° C. for 1 to 48 hours to give a compound of the formula:

[Chemical 4] To obtain the cyanoethyl compound [III]. Here, the relationship between n and m is set so that 1 ≦ m ≦ n−1, and the obtained cyanoethyl compound [III] has (n−m), ie, 1 or more in the molecule. The hydroxyl group remains.

Examples of the polyhydroxyl compound [II] include ethylene glycol, propylene glycol, 1,3-propanediol, 1,4-butanediol, neopentyl glycol, diethylene glycol,
Triethylene glycol, bisphenol A, hydrogenated bisphenol A, 1,4-dimethylolcyclohexane,
Glycerin, 1,1,1-trimethylolpropane, sorbitol, glucose, pentaerythritol and the like can be mentioned, with glycerin and pentaerythritol being particularly preferable.

Next, the above cyanoethyl compound [III]
(N−m) mol of acrylic acid or methacrylic acid based on the residual hydroxyl groups of
The cyanoethylated monomer [I] is obtained by performing an esterification reaction (dehydration reaction) under conditions of 0 to 150 ° C. and 4 to 48 hours.

The UV polymerization initiator used in the present invention is not particularly limited, and examples thereof include commonly used benzoin ether type, benzophenone type, benzoin type, ketal type, acetophenone type, thioxanthone type and the like. The amount to be compounded is usually about 0.
05-10 parts can be used, but the optimum amount is about 0.1-5 parts. If the amount is less than this, insufficient curing is likely to occur, and if it is too large, increase in dielectric loss or coloring (especially organic Dispersion type EL device) and mechanical strength reduction due to molecular weight reduction (particularly solid electrolyte) tend to cause problems and tend to be undesirable.

The UV-curable high dielectric composition according to the present invention comprises the above-mentioned cyanoethylated monomer [I] and a UV polymerization initiator, and may further have, for example, dielectric properties (dielectric constant, dielectric loss) as necessary. ) And its temperature characteristics (temperature dependence) or frequency characteristics, hygroscopicity, mechanical strength,
Glass transition temperature, softening temperature, adhesiveness, transparency, refractive index,
For the purpose of adjusting various physical properties such as flame retardancy, other monomers such as radically copolymerizable vinyl monomers and radically reactive compounds can be blended.

Specific examples of the above-mentioned other monomers include various acrylic acid esters, methacrylic acid esters, vinyl alcohol esters, acrylic acid amides and their derivatives, methacrylic acid amides and their derivatives, styrene, vinylphenol, acrylonitrile. , Methacrylonitrile, acrylic acid, methacrylic acid, maleic anhydride, maleic acid and its esters, fumaric acid and its esters, itaconic acid and its esters, allyl alcohol and its esters, vinyl chloride, vinylidene chloride, vinyl Pyridine, vinylpyrrolidone, vinyl alkyl ethers, vinylidene fluoride, vinylidene cyanide, monovinyl compounds such as styrene sulfonic acid, divinylbenzene, polyhydric alcohols to polyhydroxyl compounds Acrylates, allyl alcohol esters of polybasic acids, vinyl alcohol esters of polybasic acids, polyvinyl compounds such as allyl (meth) acrylate, and compounds having one or more mercapto groups in the molecule, disulfide compounds and the like. Of these, one or more may be used depending on the intended use. The amount to be used may be usually selected within the range of 50% (% by weight, the same applies hereinafter) of all the monomers.

The organic dispersion-type EL device according to the present invention is characterized by using the above-mentioned UV-curable high dielectric composition as a binder for each of the reflective insulating layer and the light-emitting layer therein, and a specific manufacturing method. (I) A dispersion of the above-mentioned UV-curable high-dielectric composition and inorganic high-dielectric material powder (eg titanium oxide, barium titanate, barium zirconate, barium stannate, strontium titanate powder) on the back electrode. (Hereinafter referred to as a dispersion for a reflective insulating layer) is applied and irradiated with ultraviolet rays to form a reflective insulating layer, and then the ultraviolet curable high dielectric composition and phosphor powder (for example, zinc sulfide) are formed on the reflective insulating layer. Cu and Mn, Al, Cl, Br or the like as an activator and baked on zinc selenide or the like, and a dispersion (hereinafter referred to as a dispersion for a light emitting layer) of the composition is coated and irradiated with ultraviolet rays. After forming the optical layer, the transparent electrodes are overlapped and thermocompression-bonded, or (ii) the reflective insulating layer is formed on the back electrode in the same manner as in (i) above, and then the light emitting layer is formed on the reflective insulating layer. Disperse the dispersion and overlay it with a transparent electrode and press at room temperature, or apply the dispersion of the UV curable high dielectric composition and phosphor powder on the transparent electrode side, and overlay on the reflective insulating layer and press at room temperature. Then, ultraviolet rays are irradiated from above the transparent electrode, or (iii) a reflective insulating layer and a light emitting layer are separately formed on each of the back electrode and the transparent electrode by the same method as (i) above, and then the back electrode is formed. A method of thermocompression bonding both electrodes so that the reflective insulating layer and the light emitting layer of the transparent electrode face each other. Although any of the methods (i) to (iii) can be carried out, the method (ii) does not require heating, the pressure for pressure bonding may be low pressure, is economical, and causes a failure due to heat (for example, a transparent electrode). It is preferable because problems such as wrinkles and warpage due to heat deformation and heat shrinkage of the polyester (PET) film used for the side can be avoided.

The polymer ion conductive material according to the present invention is
The above-mentioned UV-curable high-dielectric composition is used as a matrix resin, and specifically, it is composed by mixing an electrolyte salt and a low-molecular-weight polar compound into the matrix resin. It has electrical conductivity and mechanical strength.

[0018] Examples of the above-mentioned electrolyte salt, ClO ₄ ^-, B
F ₄ ⁻ , SCN ⁻ , Cl ⁻ , Br ⁻ , I ⁻ , AsO ₆ ⁻ , CF ₃
COO ⁻ , CF ₃ SO ₃ ^{− and} other anions, and Li ⁺ , K ⁺ , N
Examples thereof include alkali metal to alkaline earth metal cations such as a ⁺ and Mg ⁺⁺ and organic cations such as (CH ₃ ) ₄ N ⁺ and (C ₄ H ₉ ) ₄ N ⁺ .

Examples of the low molecular weight polar compounds include propylene carbonate, ethylene carbonate, sulfolane, N, N-
Dimethylformamide, N, N-dimethylacetamide, 2-methyltetrahydrofuran, γ-butyrolactone, dimethyl sulfoxide, succinonitrile, benzonitrile, dioxane, trioxane, glymes such as diethylene glycol dimethyl ether, acetonitrile, N-methyl-2-pyrrolidone, In addition to N, N, N ', N'-tetramethylurea, etc., ethylene glycol, diethylene glycol, triethylene glycol, propylene glycol, butanediol, neopentyl glycol, glycerin, trimethylolpropane, pentaerythritol, glucose, sorbitol Cyanoethyl ether compounds of polyhydroxyl compounds such as In addition, among these low molecular weight polar compounds, the cyanoethyl ether compound of the polyhydroxyl compound which is not commercially available is the same method as the above cyanoethylated monomer [I], that is, the reaction of the polyhydroxyl compound and acrylonitrile in the presence of the reaction catalyst. Can be easily obtained.

The amounts of the above-mentioned electrolyte salt and low-molecular polar compound to be blended should be determined depending on the conditions such as their kind, necessary conductivity, mechanical strength, and operating temperature range.
Approximately 1 electrolyte salt to 100 parts of high dielectric matrix resin
-30 parts, and about 10-90 parts of the low molecular weight polar compound are suitable, and it is preferable to dissolve the required amount of the electrolyte salt in advance with the low molecular weight polar compound before blending. In the blending amount of both components, if the amount is less than the above lower limit value, sufficient conductivity cannot be obtained, and if it exceeds the upper limit value, rather, decrease in conductivity or mechanical strength, precipitation of electrolyte salt, etc. occur. Not preferable. The electrolyte and the low molecular weight polar compound may be used alone or in combination of two or more.

[0021]

As described above, according to the present invention, in the organic dispersion type EL device, there is no harmful effect of using an organic solvent as in the conventional case,
In addition, the fear of occurrence of defects in terms of quality is eliminated, and excellent ionic conductivity and mechanical strength can be obtained in the polymer ion conductive material. Since the cyanoethylated monomer [I] used in the present invention has a relatively large molecular weight,
Low volatility, high workability during processing such as coating, and high safety for the human body.

[0022]

EXAMPLES The present invention will be described in detail with reference to Examples and Comparative Examples. Example 1 (1) Preparation of cyanoethylated monomer A: -To 136.15 g (1 mol) of pentaerythritol, 188 g of 4% sodium hydroxide solution was added, and stirred in a four-necked flask. Acrylonitrile 164.1g (3
Mol) is added dropwise, and the Michael addition reaction is completed while adjusting the reaction temperature to 40 to 45 ° C. After the reaction, the mixture was transferred to a separating funnel, washed with water, then extracted with methylene chloride, and 59 g (0.2 mol) of a cyanoethyl compound obtained by distilling off methylene chloride to 52 g (0.6 mol) of methacrylic acid and p-toluene. 3.2 g of sulfonic acid, 0.03 g of hydroquinone and 200 benzene as a polymerization inhibitor
After adding g and performing an ester reaction under reflux, excess methacrylic acid is washed off with water to obtain a cyanoethylated monomer A. The cyanoethylated monomer A contains IR and NM
Identification was confirmed using R.

(2) Production of cyanoethylated monomer B:
In the production of (1) above, a cyanoethylated monomer B is obtained in the same manner, except that the esterifying agent for the cyanoethyl compound is changed from methacrylic acid to acrylic acid.

(3) Preparation of UV-curable high dielectric composition:
-To 10 parts of the above cyanoethylated monomers A and B,
UV polymerization initiator Irgacure # 651 (manufactured by Ciba-Geigy Co., benzyl dimethyl ketal) (0.1 part) was added, and 6
Two kinds of UV-curable high dielectric compositions are obtained by dissolving under stirring at 0 ° C. under heating. After coating these on a 1 mm thick aluminum plate and irradiating them with ultraviolet rays from a high pressure mercury lamp (80 W / cm) to form a film of about 100 μm thickness, aluminum is further vacuum-deposited on the cured film, and an LCZ meter is used. When the dielectric constant at a frequency of 1 KHz was measured, it was 19.6 for cyanoethylated monomer A and 22. for B.
It was 3. By the way, the dielectric constant of the ordinary commercially available ultraviolet curable resin (epoxy acrylate, 3002M, manufactured by Kyoeisha Yushiki Kagaku Kogyo KK) was measured in the same manner, and it was 3.8.

Example 2 (Organic dispersion type EL device) To 100 parts of cyanoethylated monomer A was added 1 part of an ultraviolet polymerization initiator Irgacure # 651 (manufactured by Ciba-Geigy, benzyl dimethyl ketal), and the mixture was stirred at 60 ° C. under heating.
Dissolve completely. To this solution, 200 parts of barium titanate powder (BT-100 manufactured by Fuji Titanium Industry Co., Ltd.) previously dried in a hot air oven for 3 hours at 150 ° C. was blended, kneaded with three rolls, and deaerated under reduced pressure. After, 50mm x 100mm
Screen printing on a 0.1 mm thick aluminum sheet, then using a high pressure mercury lamp (80 W / cm),
Ultraviolet irradiation was performed at an energy density of 250 mj / cm ² to form a reflective insulating layer. Furthermore, on this reflective insulating layer, 200 parts of phosphor powder (Cu-doped ZnS manufactured by Sylvania Co., Ltd.) previously dried in a hot air oven for 3 hours at 150 ° C. and 101 parts of the same solution of cyanoethylated monomer A and UV polymerization initiator as above. Was mixed and kneaded with three rolls, deaerated under reduced pressure, screen-printed, and then irradiated with ultraviolet rays to form a light-emitting layer, as in the case of the reflective insulating layer. Next, the light emitting layer surface and the conductive side surface of a transparent conductive film (manufactured by Toray Industries, Inc., High Beam 75L-CF97) as a transparent electrode are thermocompression bonded at a temperature of 150 ° C. and a pressure of 6 kg / cm ² to form an organic dispersion type. An EL device was produced. This organic dispersion type E
When a sine wave having an effective value of 100 V and a frequency of 1 KHz was applied to the L element and luminance was measured, light emission of 65 candela / m ² was observed.

Example 3 The steps up to formation of the reflective insulating layer were performed in the same manner as in Example 2, the light emitting layer was screen-printed on the transparent electrode side, and the transparent insulating layer was laminated with the reflective insulating layer without being irradiated with ultraviolet rays to form a 1 mm thick glass plate. It was used to press the transparent conductive film from the surface side and irradiate it with ultraviolet rays.
Since the ultraviolet irradiation was performed through the glass plate and the transparent conductive film, the same high-pressure mercury lamp was used and the irradiation was performed at 50 mj / cm ² . When the luminance of the obtained organic dispersion-type EL device was measured under the same conditions as in Example ² , light emission of 78 candela / m ² was observed.

COMPARATIVE EXAMPLE 1 Conventionally, a binder resin having a high dielectric constant, which has been used in an organic dispersion type EL device, is a polymer and cannot be UV-cured. Therefore, as a comparative example, epoxy acrylate, which is a widely used ultraviolet curable resin, was used. However, an attempt was made to compare an epoxy acrylate resin (Kyoeisha Yushi Kagaku Kogyo Co., Ltd., epoxy ester 3002M) by the method of Examples 2 and 3, but because the viscosity of the epoxy acrylate was high, the screen of the reflective insulating layer and the light emitting layer was screened. Printing was not possible, and 20% of cellosolve acetate (organic solvent) was unavoidably added. Therefore, 12
After performing solvent drying at 0 ° C. for 60 minutes, ultraviolet irradiation was performed to prepare an organic dispersion-type EL device by the method of Example 2, and the brightness was measured in the same manner. As a result, almost 3 to 4 candela / m ² was obtained. No luminescence could be observed. From the results of Examples 2 and 3 and Comparative Example 1 described above, the organic dispersion type EL device using the ultraviolet curable high dielectric composition of the present invention has a great merit in the manufacturing method and is excellent in its characteristics. I understand.

Example 4 (Polymer type ionic conductive material) Cyanoethylated monomer B 10 parts, 1,6-hexanediol diacrylate 0.2 part, UV polymerization initiator Darocur 1116 (Merck acetophenone type)
1 part was mixed, and 10 parts of propylene carbonate, which is a low molecular weight polar compound, was mixed with a solution of 5 parts of lithium perchlorate as an electrolyte salt under heating, and then applied to an aluminum plate having a thickness of 1 mm at a thickness of 1 mm. The high pressure mercury lamp (80W
/ Cm) was used for curing (the propylene carbonate, which is a low molecular weight polar compound, remains after the ultraviolet curing, and the cured film is flexible but shows strong elasticity). After curing, an aluminum foil was adhered as a measuring electrode, and the resistivity at 1 KHz and 20 ° C. was measured with an LCZ meter to convert it into conductivity.
The value of 3 × 10 ⁻⁴ Siemens (S) is shown.

Comparative Example 2 To 10 parts of a random block polymer (average molecular weight 3000, hydroxyl value 56.1) consisting of ethylene oxide and propylene oxide starting from glycerin,
A mixed solution prepared by adding 20 parts of a 10% strength solution of lithium ethyl perchlorate in methyl ethyl ketone previously dissolved is dehydrated with molecular sieves, and 1.3 parts of 4,4′-diphenylmethane diisocyanate is added and dissolved. 1 of this mixture
Apply it to a 1mm thick aluminum plate at 80 ° C,
After solvent drying and curing for 2 hours, adhere aluminum foil as a measuring electrode, and use an LCZ meter for 1 KH.
When the resistivity at z and 20 ° C. was measured and converted into conductivity, the value was 6.8 × 10 ⁻⁶ S. Prior to the experiment of this example, lithium perchlorate was used as a propylene carbonate solution in the same manner as in Example 4, and an attempt was made to add the same amount to the random block polymer, but the mechanical properties after curing were remarkably poor ( It was brittle) and could not be put to practical use at all. From the results of Example 4 and Comparative Example 2 described above, it can be seen that the use of the ultraviolet-curable high dielectric composition of the present invention makes it possible to obtain a polymer-based ionic conductive material having excellent ionic conductivity and mechanical properties.

[Procedure amendment]

[Submission date] June 10, 1993

[Procedure Amendment 1]

[Document name to be amended] Statement

[Correction target item name] 0020

[Correction method] Change

[Correction content]

The amounts of the above-mentioned electrolyte salt and low-molecular polar compound to be blended should be determined depending on the conditions such as their kind, necessary conductivity, mechanical strength, and operating temperature range.
Approximately 1 electrolyte salt to 100 parts of high dielectric matrix resin
-30 parts, and about 10-900 parts of the low molecular weight polar compound are suitable, and it is preferable that the required amount of electrolyte salt is dissolved in advance with the low molecular weight polar compound before blending. In the blending amount of both components,
In either case, if the amount is less than the lower limit, sufficient conductivity cannot be obtained, and if the amount exceeds the upper limit, the conductivity is lowered, the mechanical strength is lowered, and the electrolyte salt is precipitated, which is not preferable. The electrolyte and the low molecular weight polar compound may be used alone or in combination of two or more.

[Procedure Amendment 2]

[Document name to be amended] Statement

[Name of item to be corrected] 0025

[Correction method] Change

[Correction content]

Example 2 (Organic dispersion type EL device) To 100 parts of cyanoethylated monomer A was added 1 part of an ultraviolet polymerization initiator Irgacure # 651 (manufactured by Ciba-Geigy, benzyl dimethyl ketal), and the mixture was stirred at 60 ° C. under heating.
Dissolve completely. To this solution, 200 parts of barium titanate powder (BT-100, manufactured by Fuji Titanium Industry Co., Ltd.) previously dried in a hot air oven at 150 ° C. for 3 hours was mixed, kneaded with three rolls, and deaerated under reduced pressure. After, 50mm x 100mm
Screen printing on a 0.1 mm thick aluminum sheet, then using a high pressure mercury lamp (80 W / cm),
Ultraviolet irradiation was performed at an energy density of 250 mj / cm ² to form a reflective insulating layer. Further, on this reflective insulating layer, 200 parts of phosphor powder (Cu-doped ZnS manufactured by Sylvania Co., Ltd.) previously dried in a hot air oven for 3 hours at 150 ° C. and 100 parts of the same solution of cyanoethylated monomer A and UV polymerization initiator as above. Was mixed and kneaded with three rolls, deaerated under reduced pressure, screen-printed, and then irradiated with ultraviolet rays to form a light-emitting layer, as in the case of the reflective insulating layer. Next, this light emitting layer surface and the conductive side surface of a transparent conductive film (manufactured by Toray Industries, Inc., High Beam 75L-CF97) as a transparent electrode are thermocompression bonded at a temperature of 150 ° C. and a pressure of 6 kg / cm ² to form an organic dispersion type. An EL device was produced. This organic dispersion type E
When a sine wave having an effective value of 100 V and a frequency of 1 KHz was applied to the L element and luminance was measured, light emission of 65 candela / m ² was observed.

[Procedure 3]

[Document name to be amended] Statement

[Correction target item name] 0026

[Correction method] Change

[Correction content]

Example 3 The steps up to formation of the reflective insulating layer were performed in the same manner as in Example 2, the light emitting layer was screen-printed on the transparent electrode side, and the transparent insulating layer was laminated with the reflective insulating layer without being irradiated with ultraviolet rays to form a 1 mm thick glass plate. It was used to press the transparent conductive film from the surface side and irradiate it with ultraviolet rays.
Since the ultraviolet irradiation was performed through the glass plate and the transparent conductive film, the same high pressure mercury lamp was used and the irradiation was set to 500 mj / cm ² . When the luminance of the obtained organic dispersion-type EL device was measured under the same conditions as in Example ² , light emission of 78 candela / m ² was observed.

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Claims (9)

[Claims] 1. The formula: (In the formula, 1 ≦ m ≦ n−1, m is 1 to 3, R ¹ is H or CH ₃ , and R ² has at least one of an oxygen atom, a phenylene group, a hydrogenated phenylene group and an amino group. A cyanoethylated monomer [I] represented by a certain linear or branched alkylene group); and a UV polymerization initiator. 2. The ultraviolet curable high dielectric composition according to claim 1, wherein 0.1 to 5 parts by weight of an ultraviolet polymerization initiator is added to 100 parts by weight of the cyanoethylated monomer [I]. 3. The ultraviolet-curable high dielectric composition according to claim 1, wherein another monomer copolymerizable with the cyanoethylated monomer [I] is used in combination at a ratio of 50% by weight or less based on all monomers. 4. An organic dispersion-type electroluminescence device comprising a back electrode, a reflective insulating layer, a light emitting layer and a transparent electrode which are laminated in this order, as a binder for each of the reflective insulating layer and the light emitting layer. An organic dispersion-type electroluminescence device comprising the ultraviolet-curable high-dielectric composition described in 1. 5. The method for producing an organic dispersion-type electroluminescent device according to claim 4, wherein (i) the back electrode comprises the ultraviolet-curable high dielectric composition according to claim 1 and an inorganic high dielectric material powder. After coating the dispersion and irradiating it with ultraviolet rays to form a reflective insulating layer, the dispersion of the ultraviolet-curable high dielectric composition according to claim 1 and phosphor powder is overlaid on the reflective insulating layer and irradiated with ultraviolet rays. After forming the light emitting layer, the transparent electrodes are superposed and thermocompression-bonded, or (ii) a dispersion of the ultraviolet curable high dielectric composition and the inorganic high dielectric material powder according to claim 1 on the back electrode. And irradiating with ultraviolet rays to form a reflective insulating layer, and then the dispersion of the ultraviolet-curable high dielectric composition according to claim 1 and phosphor powder is applied on the reflective insulating layer, and a transparent electrode is applied to the dispersion. And then press at room temperature, or claim on the transparent electrode side. 1. The dispersion of the UV-curable high-dielectric composition and the phosphor powder described in 1 is applied, superposed on the reflective insulating layer and press-bonded at room temperature, and ultraviolet rays are irradiated from above the transparent electrode, or (iii) the back electrode is charged. Item 2. A dispersion of the ultraviolet-curable high-dielectric composition according to item 1 and a powder of an inorganic high-dielectric material is applied and irradiated with ultraviolet rays to form a reflective insulating layer, and on the other hand, the transparent electrode is ultraviolet-cured according to claim 1. After applying a dispersion of highly conductive high dielectric composition and phosphor powder and irradiating ultraviolet rays to form a light emitting layer, both electrodes are thermocompression bonded so that the reflective insulating layer of the back electrode and the light emitting layer of the transparent electrode face each other. A method for manufacturing an organic dispersion-type electroluminescence device, which comprises: 6. The ultraviolet-curable high dielectric composition according to claim 1, which is used for forming a dielectric film of a film capacitor by applying a thin film on a metal foil and then irradiating with an ultraviolet ray. 7. A polymer ion conductive material comprising the ultraviolet curable high dielectric composition according to claim 1 as a matrix resin. 8. The polymer ion conductive material according to claim 7, wherein the matrix resin is mixed with an electrolyte salt and a low molecular weight polar compound. 9. The polymer-based ionic conductive material according to claim 7, which is cured by irradiation with ultraviolet rays.