JP2010080292A - Double-sided light-emitting type organic electroluminescent panel, and its manufacturing method - Google Patents

Abstract

<P>PROBLEM TO BE SOLVED: To provide a double-sided light-emitting type organic electroluminescent panel in which the deterioration of an organic EL element is suppressed, and its manufacturing method. <P>SOLUTION: In the double-sided light-emitting type electroluminescent panel having a first substrate 1, a first organic electroluminescent element 2 arranged on the substrate, a second substrate 3, and a second organic electroluminescent element 4 arranged on the substrate so that the first and the second organic electroluminescent elements oppose each other, the double-sided light-emitting type organic EL panel has a filling layer 5 arranged between and at the surrounding of the first and the second organic electroluminescent elements, and a sealing layer 6 arranged in a frame shape at the surrounding of the filling layer in contact with the first substrate and the second substrate. The filling layer contains a thermoplastic rubber component as a main component, and the sealing layer contains a cured resin as a main component. <P>COPYRIGHT: (C)2010,JPO&INPIT

Description

  The present invention relates to a double-sided light emitting organic electroluminescence panel and a method for manufacturing the same.

  In recent years, with the diversification of information equipment, there has been an increasing need for flat display elements that consume less power than commonly used CRTs (cathode ray tubes). As one of such flat display elements, an organic electroluminescence (hereinafter abbreviated as “organic EL”) element having features such as high efficiency, thinness, light weight, and low viewing angle dependency has attracted attention. There are active developments in the display using the.

  The organic EL element injects electrons and holes from the electron injection electrode and the hole injection electrode into the light emitting part, recombines the injected electrons and holes at the emission center to bring the organic molecules into an excited state, and the organic molecules Is a self-luminous element that emits fluorescence when it returns from the excited state to the ground state.

  When the organic EL element is driven for a certain period, there is a problem that light emission characteristics such as light emission luminance, light emission efficiency, and light emission uniformity are significantly deteriorated as compared with the initial case. The causes of such deterioration of the light emission characteristics include oxidation of the electrode due to oxygen that has entered the organic EL element, oxidative decomposition of the organic material due to heat generation during driving, and the electrode due to moisture in the air that has entered the organic EL element Examples thereof include oxidation and modification of organic substances. Furthermore, the interface of the structure peels off due to the influence of oxygen and moisture, the heat generation during driving and the environment during driving are high temperature, etc. Mechanical deterioration of the structure, such as stress generated at the interface of the body and peeling of the interface, can also be cited as a cause of the deterioration of the light emission characteristics.

  In order to suppress such a problem, the technique which seals an organic EL element and suppresses a contact with a water | moisture content or oxygen is examined. For example, Patent Document 1 describes a technique in which when a hermetic space is formed by a substrate and a shield member, both are bonded with a cationic curing type ultraviolet curing epoxy resin adhesive. Patent Document 2 describes a technique in which a flexible film on which a gas barrier layer is formed is coated on the outer surface of an organic EL element as a sealing substrate. Patent Document 3 discloses a technique for bonding a substrate and a sealing plate through a sealing agent in a reduced-pressure atmosphere, and then curing the sealing agent, and an organic electroluminescent element with a low-viscosity first sealing. It describes a technique of sealing with a stopper and sealing with a high-viscosity sealant containing a filler so as to surround the organic electroluminescence element. Further, Patent Document 4 discloses a light having a structure in which an electronic component is sealed by a sealant layer including an uncured surface sealant portion and an uncured outer frame sealant portion surrounding the surface sealant portion. A device manufacturing method is described. Patent Document 5 describes an organic EL device having an adhesive film including an adhesive sealing composition having a hydrogenated cyclic olefin polymer and a polyisobutylene having a weight average molecular weight of 500,000 or more. ing.

  On the other hand, a transparent organic EL element has attracted attention and has been developed as an organic EL panel capable of displaying light on both sides. An organic EL panel capable of simultaneously displaying completely different independent images and character information on both the front and back surfaces is disclosed in Patent Document 6, for example. Patent Document 7 discloses a double-sided light emitting display panel formed by bonding two organic EL elements back to back.

JP-A-10-233283 Japanese Patent No. 4010394 JP 2004-265615 A JP 2006-244978 A JP 2007-197517 A JP 2005-267926 A JP 2006-039554 A

  However, the conventional techniques as described above are still not sufficient from the viewpoint of suppressing the deterioration of the element. If this reason is presumed, in these conventional techniques, since the curable resin such as epoxy is used in the upper part and the peripheral part (side surface part) of the organic electroluminescence element, it is included in the curable resin. A highly reactive component such as a curing agent adversely affects the portion in contact with the organic electroluminescence element, causing deterioration of the element. In Patent Document 5, a curable resin is not used as a sealant for an organic electroluminescence element, but a hydrogenated cyclic olefin polymer used as a sealant and a weight average molecular weight of 500,000 or more. It can be mentioned that the gas barrier property is insufficient only with the adhesive sealing composition having polyisobutylene having a cause of deterioration of the device.

  On the other hand, in a double-sided light emitting EL element, when a space between two organic light emitting layers is used as a sealed space as disclosed in Patent Document 7, it is desired to make the panel flexible and reduce the thickness of the panel. In addition, it is difficult to stably hold the shape, and there is a problem that the element is easily deteriorated due to an impact or the like, or the elements collide with each other to cause a short circuit.

  This invention is made | formed in view of the said actual condition, The objective of this invention is providing the double-sided emission type organic electroluminescent panel in which deterioration of the organic electroluminescent element was suppressed, and its manufacturing method.

  An organic electroluminescence panel according to the present invention includes a first substrate, a first organic electroluminescence element disposed on the substrate, a second substrate, and a second organic electroluminescence disposed on the substrate. In a double-sided light emitting electroluminescence panel having a luminescence element so that the first and second organic electroluminescence elements face each other, a filling disposed between and around the first and second organic electroluminescence elements And a sealing layer arranged in a frame shape around the filling layer in contact with the first substrate and the second substrate, the filling layer having a thermoplastic rubber component as a main component. It is a double-sided emission type organic electroluminescent panel which contains and the said sealing layer contains curable resin as a main component.

  In the present invention, a filler layer containing a thermoplastic rubber component as a main component is disposed on and around the first and second organic electroluminescence elements, and the filler layer is disposed in the first and second layers. Since it has the structure sealed with the base | substrate and the sealing layer which has curable resin as a main component, the double-sided emission type organic electroluminescent panel in which deterioration of the organic electroluminescent element was suppressed can be provided.

Further, the present invention provides a step of preparing a first organic electroluminescence element disposed on the first substrate,
Providing a second organic electroluminescent element disposed on the second substrate;
The second organic electroluminescence element on the second substrate is exposed so that the peripheral portion of the surface on which the element of the second substrate is disposed is exposed in the filling layer containing the thermoplastic rubber component as a main component. Forming a laminated body a by laminating on and around the substrate;
The first organic electroluminescence is arranged on the first substrate so that the filling layer of the laminated body a is disposed on and around the first organic electroluminescence element. Laminating on the element to form a laminate b;
A curable resin composition is applied around the filling layer so as to seal between the first substrate and the second substrate in the laminate b, and a curing reaction is performed to form a sealing layer. There is also provided a method for producing a double-sided light emitting organic electroluminescence panel having the steps.

  In the method of manufacturing an organic electroluminescence panel according to the present invention, in the step of forming the laminate a, the filling layer may be melted without using a solvent and laminated on the second substrate. preferable. In such a case, since there is essentially no residual solvent in the filling layer, deterioration of the element due to the residual solvent is prevented even when it comes into contact with the organic electroluminescent element.

  In the organic electroluminescence panel and the method for producing the same according to the present invention, the packed layer includes an ABA type styrene block copolymer rubber and / or a hydride thereof of 50 to 100% by weight, and an AB type. A styrene block copolymer rubber and / or a hydride thereof containing 0 to 50% by weight of a rubber component, and containing 50 parts by weight or more tackifying resin as a main component with respect to 100 parts by weight of the rubber component, This is preferable from the viewpoint of suppressing deterioration of the element.

  In the organic electroluminescence panel and the method for producing the same according to the present invention, the packed layer includes a styrene-isoprene-styrene block copolymer rubber, a styrene-butadiene-styrene copolymer rubber, a styrene-ethylene-butylene-styrene copolymer. It is preferable from the point of suppression of deterioration of an element to contain 1 type or more selected from the group which consists of united rubber and styrene-ethylene-propylene-styrene copolymer rubber.

  In the organic electroluminescence panel and the manufacturing method thereof according to the present invention, the ABA type styrene block copolymer rubber or the hydride thereof in the packed layer is 10 to 40 mol%. This is preferable from the viewpoint of suppressing deterioration of the element.

  In the organic electroluminescence panel and the manufacturing method thereof according to the present invention, it is preferable from the viewpoint of suppressing deterioration of the element that the filling layer does not contain a curing agent.

  In the organic electroluminescence panel and the manufacturing method thereof according to the present invention, the tackifying resin in the packed bed is at least one selected from the group consisting of hydrogenated petroleum resins, rosin resins, and terpene resins. It is preferable from the viewpoint of suppressing deterioration of the element and transparency.

  In the organic electroluminescence panel and the manufacturing method thereof according to the present invention, the filling layer preferably contains a getter agent from the viewpoint of suppressing deterioration of the element.

  In the organic electroluminescence panel and the method for producing the same according to the present invention, it is preferable to further have a getter layer from the viewpoint of suppressing deterioration of the element.

  In the organic electroluminescence panel and the manufacturing method thereof according to the present invention, it is preferable that the sealing layer contains an epoxy resin as a main component from the viewpoint of suppressing deterioration of the element due to moisture resistance and application workability. .

  In the organic electroluminescence panel and the manufacturing method thereof according to the present invention, even if the first substrate and / or the second substrate have flexibility, they can be suitably used.

  In the organic electroluminescent panel and the manufacturing method thereof according to the present invention, it is preferable that a barrier layer is provided between the organic electroluminescent element and the filling layer from the viewpoint of suppressing deterioration of the element.

  In the organic electroluminescence panel and the manufacturing method thereof according to the present invention, a plurality of first organic electroluminescence elements arranged on the first substrate at a predetermined interval on the first substrate, and the second substrate. And a plurality of second organic electroluminescent elements arranged in a plane at a predetermined interval, at least a first non-light-emitting portion existing between the plurality of first organic electroluminescent elements, The second organic electroluminescence element is opposed to the second organic electroluminescence element, and the second non-light emitting portion and the first organic electroluminescence element are present between the plurality of second organic electroluminescence elements. It may be an aspect possessed by. In the case of such an aspect, there is an advantage that the resolution of the obtained organic EL panel can be doubled and a sense of depth can be expressed.

According to the present invention, the filling layer containing the thermoplastic rubber component as a main component is disposed on and around the first and second organic electroluminescence elements, and the filling layer is disposed in the first and second layers. Therefore, it is possible to provide a double-sided light emitting organic electroluminescence panel in which deterioration of the organic electroluminescence element is suppressed.
According to the present invention, the first and second bases, the first and second organic electroluminescence elements, and the sealing layer are formed by the filling layer containing the thermoplastic rubber component as a main component as described above. By filling the space, even if the panel is thinned or a flexible substrate is used, the filling layer is highly elastic, so it can be deformed when used or deformed by impact. The organic EL layer has a function of stably holding the shape, and can suppress the occurrence of scratches and cracks in the organic EL layer. Further, since the insulating filler layer is interposed between the two organic EL elements, it is possible to prevent the elements from colliding with each other and causing a short circuit.

  Further, according to the present invention, the organic EL element on the other substrate is also sealed using the laminate a in which a specific filling layer is laminated on and around the organic EL element on one substrate, In order to seal between the first and second substrates, a curable resin composition is applied around the filling layer, and a curing reaction is performed to form a sealing layer. A double-sided light emitting organic electroluminescence panel in which deterioration of the element is suppressed can be manufactured.

I. Double-sided light-emitting organic electroluminescence panel A double-sided light-emitting organic electroluminescence panel according to the present invention includes a first substrate, a first organic electroluminescence element disposed on the substrate, a second substrate, and the substrate. In the double-sided light emitting type electroluminescence panel having the second organic electroluminescence element disposed above so that the first and second organic electroluminescence elements face each other, the first and second organic electroluminescence elements A filling layer disposed between and around the element; and a sealing layer disposed in a frame shape around the filling layer in contact with the first substrate and the second substrate, However, it contains a thermoplastic rubber component as a main component, and the sealing layer contains a cured resin as a main component.
Here, the thermoplastic rubber component is a so-called thermoplastic elastomer, which is not vulcanized or cross-linked and has characteristics similar to vulcanized rubber at the use temperature such as room temperature. It refers to a polymer or polymer blend that disappears and can be easily processed, and that when it is returned to the working temperature, it exhibits its original properties again.

In the present invention, on the first and second organic EL elements and around the first and second organic EL elements, a filling layer containing the thermoplastic rubber component as a main component as described above is disposed, The first and second organic EL elements are covered with a filling layer. The filling layer used in the present invention is essentially non-curable without containing a curing component, moisture, or the like that adversely affects the element. In addition, as the packed bed of the present invention, one that can be heated and melted without using a solvent can be selected. In the present invention, such a filling layer has a structure in which the first and second organic EL elements are covered on the entire periphery and side surfaces (side surfaces). The moisture resistance of the element can be improved while preventing the element from being deteriorated due to a highly reactive component such as an agent or a residual solvent.
In this invention, it has the structure which sealed the organic EL element covered with the said filling layer by the 1st and 2nd base | substrate and the sealing layer which has cured resin as a main component. As described above, the organic EL element is first coated with a relatively soft component filling layer, and further sealed with a relatively hard component sealing layer having a high gas barrier property, thereby sealing the element against oxygen and moisture. Therefore, it is possible to provide an organic electroluminescence panel in which deterioration of the element can be suppressed.

Hereinafter, the organic EL panel of the present invention will be described. FIG. 1 shows an example of the organic EL panel of the present invention. In this example, on the first substrate 1, the first organic EL element 2 disposed on the substrate 1, the second substrate 3, and the second organic EL disposed on the substrate 3. The element 4 is disposed so that the first and second organic EL elements (2, 4) face each other, and is disposed between and around the first and second organic EL elements (2, 4). The sealing layer 6 arranged in a frame shape around the filling layer 5 is formed in contact with the filling layer 5 and the first base 1 and the second base 3.
The first base, the first organic EL element, the second base, and the second organic EL element may be any one of the two opposing bases and the two organic EL elements. One of them is the first substrate and the first organic EL element, and the other is the second substrate and the second organic EL element.
Hereinafter, each element which comprises such an organic electroluminescent panel of this invention is demonstrated concretely.

1. Filling Layer One of the features of the present invention is that, as described above, the filling layer containing a thermoplastic rubber component as a main component is disposed on and around the first and second organic EL elements. . Note that “containing as a main component” means that the thermoplastic rubber component is contained in the total amount of the packed bed in an amount of 50% by weight or more, preferably 80% by weight or more, and more preferably 90% by weight or more.

  The thermoplastic rubber component is a component that imparts some moisture resistance, high elasticity, and flexibility to the packed layer. The rubber component as described above does not have a vulcanization step and has high strength and high flexibility and exhibits rubber elasticity at room temperature. The filling layer used in the present invention does not need to undergo a curing reaction using a curing agent, and element degradation due to the curing agent, and element degradation due to high heat and light irradiation used for the curing reaction are suppressed.

  In the present invention, the space formed by the first and second substrates, the first and second organic electroluminescence elements, and the sealing layer is filled with the above high elasticity and flexibility. Filled with layers. As a result, the organic EL panel of the present invention can easily return to its original shape even when the panel is thinned or when a flexible substrate is used, even if it is deformed by use or impact. It has a function to hold and can prevent the organic EL layer from being scratched or cracked. Further, since the filling layer made of such an insulating material is interposed between the two organic EL elements, it is possible to prevent the elements from colliding with each other and causing a short circuit.

  In the present invention, it is further preferable to combine such a rubber component with a tackifying resin from the viewpoint of imparting an appropriate viscosity and adhesiveness. In such a case, it is possible to improve the wettability and adhesion when the rubber component is hot-melted, and to adhere and cover the substrate while following the substrate and the organic EL element as the adherend.

Examples of the thermoplastic rubber component include styrene block copolymers, polybutadiene, polyisoprene, polyisobutylene, polychloroprene, ethylene-propylene-diene monomer rubber, ethylene propylene rubber, nylon elastomer, polyester elastomer, urethane elastomer, silicon elastomer. And fluorine elastomer.
As the thermoplastic rubber component, it is preferable to select a component that can be hot-melt processed at 200 ° C. or lower. In such a case, the filling layer can be laminated without using a solvent without adversely affecting the organic EL element. When it is not necessary to use a solvent when laminating on an organic EL element or when forming a filling layer, it is possible to prevent adverse effects of the residual solvent in the filling layer on the element.

  Among the packed layers, among others, ABA type styrene block copolymer rubber and / or its hydride 50 to 100% by weight, and AB type styrene block copolymer rubber and / or its hydride 0 It is preferable to contain as a main component a rubber component composed of ˜50% by weight and a tackifier resin of 50 parts by weight or more with respect to 100 parts by weight of the rubber component.

ABA type styrene block copolymer rubber and / or its hydride 50 to 100% by weight, and AB type styrene block copolymer rubber and / or its hydride 0 to 50% by weight The component can be hot melt processed at 200 ° C. or lower, so there is no need to use a solvent when laminating on an organic EL element or when forming a filling layer, and the adverse effect of residual solvent in the filling layer on the element is also prevented. it can.
As a layer covering not only the upper part of the organic EL element but also the surrounding part (side surface), when a specific rubber component or tackifying resin is combined in a specific ratio, the filling layer is directly bonded to the organic EL element. However, it is possible to particularly prevent the deterioration of the element due to the component caused by the filling layer.

In the A-B-A block copolymer rubber and the A-B block copolymer rubber, A is a styrene polymer block, B is a butadiene polymer block, an isoprene polymer block, or a vinyl-isoprene polymer block. It is. These block copolymer rubbers are styrene block copolymers having polystyrene as a hard segment. Specifically, the ABA block copolymer rubber and its hydride are styrene-butadiene-styrene block copolymer rubber (SBS), styrene-isoprene-styrene block copolymer rubber (SIS), Styrene-vinyl isoprene-styrene block copolymer rubber (SVIS), SBS hydride styrene-ethylene-butene-styrene block copolymer rubber (SEBS), SIS hydride styrene-ethylene-propylene- Styrene block copolymer rubber (SEPS). In addition, the AB type block copolymer rubber and its hydride are styrene-butadiene block copolymer rubber (SB), styrene-isoprene block copolymer rubber (SI), and styrene-ethylene which is a SB hydride. -Butene block copolymer rubber (SEB), styrene-ethylene-propylene block copolymer rubber (SEP) which is a hydride of SI.
Among them, the inclusion of styrene-isoprene-styrene block copolymer rubber and / or styrene-ethylene-propylene-styrene copolymer rubber improves the adhesion with the EL element and expands the options for the tackifying resin to be combined. To preferred.

  These A-B-A type block copolymer rubber and its hydride, and the AB-type block copolymer rubber and its hydride have a weight average molecular weight of 1,000 to 500, The weight average molecular weight of the B block part is preferably 15,000 to 1,000,000. The weight average molecular weight in the present invention is calculated based on a calibration curve prepared using a polystyrene standard material by gel permeation chromatography (GPC) measurement.

  The ABA type block copolymer rubber and the hydride thereof are those having a styrene component of less than 10% by mole because the tackiness is too high and rubber elasticity may not be exhibited. Is preferred. On the other hand, when the styrene component exceeds 40 mol%, the tackiness is too weak, and it may become hard and may not exhibit rubber elasticity.

  The AB type block copolymer rubber and its hydride, and the AB type block copolymer rubber and its hydride are, for example, Nippon Zeon Co., Ltd., Asahi Kasei Corporation, Kuraray Co., Ltd., It is marketed by JSR Corporation and is available.

The AB-A type block copolymer rubber or hydride thereof and the AB-type block copolymer rubber or hydride thereof, when the total amount of the rubber components is 100% by weight, ABA type styrene block copolymer rubber and / or its hydride 50 to 100% by weight, and AB type styrene block copolymer rubber and / or its hydride 0 to 50% by weight Used by mixing. By using such a mixing ratio, the effect of the packed bed as described above can be suitably obtained.
In particular, when the total amount of the rubber component is 100% by weight, the ABA type styrene block copolymer rubber and / or its hydride 50 to 90% by weight, and the AB type styrene block copolymer weight The combined rubber and / or hydride thereof is preferably mixed and used in the range of 10 to 50% by weight from the viewpoint of adhesion to the element substrate and the sealing substrate and the development of rubber elasticity.
The AB-A type block copolymer rubber or hydride thereof and the AB type block copolymer rubber or hydride thereof may be used in addition to using a mixture obtained by mixing the two in advance. When preparing the rubber component used in the above, it is also possible to use both in such a manner that the mixing ratio of both falls within the above range.

  On the other hand, as tackifying resins, rosin, rosin derivatives (hydrogenated rosin, disproportionated rosin, polymerized rosin, rosin ester (such as esterified rosin such as alcohol, glycerin and pentaerythritol)), terpene resin (α-pinene, β-pinene), terpene phenol resin, aromatic modified terpene resin, hydrogenated terpene resin, aliphatic petroleum resin, aromatic petroleum resin, copolymer petroleum resin, alicyclic petroleum resin, coumarone-indene resin, styrene Resin, phenol resin, xylene resin and the like.

  Among them, at least one selected from the group consisting of hydrogenated petroleum resins, rosin resins, and terpene resins has good compatibility with the specific rubber component, and can form a packed layer with excellent transparency. Are preferably used. Examples of such hydrogenated petroleum resins include water, which is a C5 petroleum resin hydration resin obtained by copolymerizing C5 fractions such as pentene, isoprene, piperine, and 1.3-pentadiene produced by thermal decomposition of petroleum naphtha. Dicyclopentadiene resin (Tonex Co., Ltd .: Escorez 5300,5400 series, Eastman Co .: Eastotac H series, etc.), partially hydrogenated aromatic modified dicyclopentadiene resin (Tonex Co., Ltd .: Escorez 5600) Series, etc.), hydrogenated C9 petroleum resin obtained by copolymerization of C9 fractions such as indene, vinyltoluene, α- or β-methylstyrene produced by thermal decomposition of petroleum naphtha (Arakawa Chemical Industries Ltd.) Company-made: Alcon P or M series), a resin obtained by hydrogenating the above-mentioned copolymer petroleum resin of C5 fraction and C9 fraction (made by Idemitsu Kosan Co., Ltd .: Lee Marv series), and the like. Among these, alicyclic saturated hydrocarbon resins are preferably used from the viewpoint of good compatibility with the specific rubber component.

The blending in the packed bed used in the present invention preferably uses 50 parts by weight or more of tackifying resin with respect to 100 parts by weight of the rubber component.
This is because if the tackifying resin is less than 50 parts by weight with respect to 100 parts by weight of the rubber component, the tackiness is too weak and it may not adhere to the EL element substrate and the sealing substrate. Especially, it is preferable that tackifying resin is used in the ratio of 50-200 weight part with respect to 100 weight part of said rubber components from the point of adhesion with an EL element substrate and a sealing substrate, and expression of rubber elasticity.

  The packed bed of the present invention can contain any additive in addition to the specific rubber component and tackifying resin as long as the effects and transparency of the present invention are not impaired. Examples of such additives include getter agents, fillers, softeners, ultraviolet absorbers, ultraviolet stabilizers, oxidation inhibitors, and resin stabilizers. As the softening agent, for example, paraffin, naphthenic oil, various waxes and the like are used.

In the present invention, the getter agent is a substance having at least a hygroscopic function, preferably also having a gas (for example, oxygen) absorption and adsorption function. As the getter agent, a hygroscopic agent, a desiccant, an oxygen absorbent and the like are used alone or in a mixed state. The getter agent may be dispersed in the packed bed, but may be locally disposed. Alternatively, the filling layer may have a multilayer structure and be dispersed only in the second filling layer that does not contact the organic EL element.
Alternatively, as shown in FIG. 2, a structure having a getter layer 7 containing a getter agent as a main component between the first organic EL element and the second organic EL element may be used.

  Examples of the getter agent include metal oxides such as calcium oxide, magnesium oxide and barium oxide, sulfates such as magnesium sulfate, sodium sulfate and nickel sulfate, and organic metal compounds such as aluminum oxide octylate.

  A getter agent may be used independently and may mix and use 2 or more types. When added, the addition amount of the getter agent is preferably 0.01 to 20% by weight based on the total amount of the packed bed.

  Examples of the filler include calcium carbonate such as calcium carbonate, magnesium carbonate, and dolomite, magnesium carbonate, kaolin, calcined clay, pyrophyllite, pentite, sericite, zeolite, talc, attapulgite, wollastonite, and the like. Silicates such as silicate, diatomaceous earth, and silica powder, barium sulfate such as aluminum hydroxide, pearlite, and precipitated barium sulfate, calcium sulfate such as gypsum, calcium sulfite, carbon black, zinc oxide, and titanium dioxide.

  These fillers preferably have an average primary particle diameter of 1 to 100 nm, and more preferably 5 to 50 nm, considering a decrease in transparency of the packed layer due to light scattering, for example. Further, when a plate-like or flake-like filler is used to further improve the low moisture permeability, the average primary particle diameter is preferably 0.1 to 5 μm. Further, from the viewpoint of dispersibility with respect to the resin, a hydrophilic filler whose surface is subjected to a hydrophobic treatment is preferably used. Hydrophobic fillers can be prepared by treating the surface of normal hydrophilic fillers with silylating agents such as n-octyltrialkoxysilane, alkyl having a hydrophobic group, aryl, aralkyl silane coupling agents, dimethyldichlorosilane, hexamethyldisilazane, etc. And polydimethylsiloxane having a hydroxyl group at the terminal, or higher alcohols such as stearyl alcohol, and those obtained by treatment with higher fatty acids such as stearic acid.

  A filler may be used independently and may be used in mixture of 2 or more types. When added, the amount of filler added is preferably 0.01 to 20% by weight based on the total amount of the packed bed.

  Examples of the ultraviolet absorber include benzotriazole compounds, oxazolic acid amide compounds, and benzophenone compounds. These compounds can usually be used in the range of about 0.01 to 3% by weight based on the total amount of the packed bed.

  Examples of UV stabilizers include hindered amine compounds. These compounds can usually be used in the range of about 0.01 to 3% by weight based on the total amount of the packed bed.

  Examples of the oxidation inhibitor include hindered phenol compounds and phosphate ester compounds. These compounds can usually be used in the range of about 0.01 to 2% by weight based on the total amount of the packed bed.

  Examples of the resin stabilizer include a phenol resin stabilizer, a hindered amine resin stabilizer, an imidazole resin stabilizer, a dithiocarbamate resin stabilizer, a phosphorus resin stabilizer, and a sulfur ester resin stabilizer. Can do.

  The thickness of the filling layer is not particularly limited as long as the first and second organic EL elements can be appropriately covered, but is usually in the range of 1 to 200 μm, preferably in the range of 3 to 100 μm, and more preferably, It is in the range of 5 to 50 μm.

2. Sealing layer In the present invention, for the purpose of improving the sealing effect of the organic EL panel, a sealing layer containing a cured resin as a main component, which is disposed around the filling layer in a frame shape, is filled. It is characterized by having in combination with a layer. “Containing as a main component” means that the cured resin is contained in the total amount of the sealing layer by 50% by weight or more, preferably 80% by weight or more, and more preferably 90% by weight or more.

  The curable resin refers to a resin cured by light and / or heat using, for example, a curable resin such as a photocurable resin and / or a thermosetting resin. Since such a cured resin has high moisture resistance, it has a characteristic that gas barrier properties are good. However, on the other hand, since the curable resin to be used contains a component having a highly reactive functional group such as a curing agent, when used in a portion in direct contact with the EL element, the deterioration of the EL element is promoted. There was a case. In the present invention, a sealing layer containing a curable resin as a main component is not directly contacted with an EL element, and is disposed around the filling layer and used for sealing, so that the EL element is deteriorated by a sealing agent. The gas barrier property is improved while suppressing the deterioration of the EL element due to their synergistic effect. Note that light includes not only electromagnetic waves having wavelengths in the visible and invisible regions, but also particle beams such as electron beams, and radiation or ionizing radiation that collectively refers to electromagnetic waves and particle beams.

  Examples of the curable resin used in the present invention include various ultraviolet curable resins, electron beam curable resins, thermosetting resins, and two-component curable resins. More specifically, thermosetting resins such as urea resin, melamine resin, phenol resin, resorcinol resin, epoxy resin, unsaturated polyester resin, polyurethane resin or acrylic resin; ester acrylate, urethane Radical type photocurable resins using resins such as various acrylates such as acrylates, epoxy acrylates, melamine acrylates, acrylic resin acrylates, or urethane polyesters; and cationic photocurable resins using resins such as epoxies and vinyl ethers. .

The curable resin used in the present invention is not particularly limited as long as it can be cured after application using a solvent-free coating solution. Preferred resins include epoxy resins such as a two-component thermosetting epoxy resin, a one-component thermosetting epoxy resin, and an ultraviolet curable epoxy resin.
More specifically, two-component epoxy resin (20X-325) manufactured by Three Bond Co., Ltd., WORLD ROCK 8723L2 manufactured by Kyoritsu Chemical Industry Co., Ltd., and the like can be given.

  The sealing layer of this invention can contain arbitrary additives in addition to the said cured resin in the range which does not impair the effect of this invention. Examples of such additives include getter agents, fillers, ultraviolet absorbers, ultraviolet stabilizers, oxidation inhibitors, and resin stabilizers as described in the above packed bed.

  The thickness of the sealing layer is not particularly limited as long as the filling layer can be appropriately covered and the first and second substrates can be sealed. Usually, the thickness is set to be the same as that of the packed layer, but may be smaller than the packed layer. For example, when at least one of the flexible substrates is used, the space between the first and second substrates may be smaller than the thickness of the filling layer. The thickness of the sealing layer is usually in the range of 1 to 200 μm, preferably in the range of 3 to 100 μm, and more preferably in the range of 5 to 50 μm.

3. First and second substrates As the first and second substrates used in the present invention, light that strongly supports the organic EL element and from which light from the organic EL layer is led out to the substrate side is used. There is no particular limitation as long as it has transparency. If the first electrode layer of the EL element described later has a necessary strength, it may be formed so as to also serve as the first electrode layer.
The first and second substrates may be the same or different in size and type.

  The base material may be a flexible material or a hard material, for example, depending on the application. Specific examples of materials that can be used include glass, polyethylene, polypropylene, polyethylene terephthalate, polymethyl methacrylate, polymethyl acrylate, polyester, and polycarbonate. As the substrate, a substrate having a high gas barrier property made of a material such as glass or resin is preferably used from the viewpoint of suppressing element deterioration due to oxygen or moisture.

As the first and second substrates, a flexible film, a resin plate, or the like is preferably used in terms of impact resistance and design properties. Further, in order to obtain a flexible organic EL panel, a flexible resin film with a gas barrier layer, a thin glass plate having a thickness of about 10 to 100 μm, and the like are used. A flexible organic EL panel is advantageous in that it can be applied to various uses.
The film thickness of the flexible film used as the substrate is usually in the range of 5 μm to 1000 μm, preferably in the range of 20 μm to 500 μm, particularly preferably in the range of 50 μm to 300 μm. If the film thickness is larger than the above range, it is highly possible that the film does not have flexibility, and the thickness of the EL element itself is increased, which is contrary to the demand for thinning. A thin film is not preferable because it may cause a problem in strength, although it depends on the material constituting the film.

  The material of such a film is not particularly limited as long as it is a material that can be formed into a film. Polyethylene, polypropylene, polyethylene terephthalate, polymethyl methacrylate, polymethyl acrylate, polyester, polycarbonate, fluorine resin , Polyvinyl chloride, polyvinyl fluoride, polystyrene, ABS resin, polyamide, polyacetal, modified polyphenylene ether, polysulfone, polyarylate, polyetherimide, polyethersulfone, polyamideimide, polyimide, polyphenylene sulfide, liquid crystalline polyester, polybutylene Terephthalate, polyethylene naphthalate, polymicroxylene dimethylene terephthalate, polyoxymethylene, polyethersulfone, poly -Ether ether ketone, polyacrylate, acrylonitrile-styrene resin, ABS resin, phenol resin, urea resin, melamine resin, unsaturated polyester resin, epoxy resin, polyurethane, silicone resin, amorphous polyolefin, inorganic thin film, etc. be able to.

  In the present invention, it is particularly preferable to use polyethylene terephthalate, polycarbonate, or polyethersulfone.

  In the present invention, the substrate is preferably a substrate in which a gas barrier layer having gas barrier properties is formed on the flexible film. Since a resin film generally has poor gas barrier properties, a resin film having a gas barrier layer formed on it is preferably used.

  Such a gas barrier layer is not particularly limited as long as it has gas barrier properties, but is preferably light transmissive. The gas barrier layer may be a single layer or a stack of a plurality of layers. Further, the formation method may be a wet method, but generally a gas barrier layer formed by a vacuum film formation method is preferably used.

Preferable materials constituting the gas barrier layer in the present invention include SiO _x , SiO _x N _y , and SiN _x . (Here, X and Y are 0 to 2.)
In the case where a resin film is used, it is preferably a film formed by sputtering or plasma CVD, and is preferably SiO _X N _Y. Further, in order to fill the pin hole of the SiO _X N _Y layer, a hybrid with an organic layer may be used.

The gas barrier properties required for the substrate used in the present invention are not particularly limited, but generally the oxygen permeability is 10 ⁻³ cc / m ² / day or less and the water vapor permeability is 10 ⁻⁶ g. / M ² / day or less is preferable.
The shape of the substrate is not particularly limited and can be appropriately selected and used.

5). 1st and 2nd organic EL element The 1st and 2nd organic EL element used for this invention is a at least light emitting layer arrange | positioned between a pair of opposing 1st electrode layer and 2nd electrode layer, and the said electrode layer And at least an organic EL layer. The organic EL element can have various configurations known in the technical field. In the organic EL panel of the present invention, not only one organic EL element but also a plurality of organic EL elements may be arranged on one base. The first and second organic EL elements may be the same or different in size and type.

FIG. 5 is a partially enlarged schematic cross-sectional view illustrating the arrangement of organic EL elements in the organic EL panel of the present invention. As shown in FIG. 5, the organic EL panel of the present invention includes a plurality of first organic EL elements 2 arranged on the first base 1 in a plane with a predetermined interval, and the second organic EL element 2. A plurality of second organic EL elements 4 arranged in a plane on the substrate 3 at a predetermined interval, and at least a first non-light emission existing between the plurality of first organic EL elements. The portion 15 and the second organic EL element 4 face each other, and the second non-light emitting portion 16 and the first organic EL element 2 existing between the plurality of second organic EL elements are The aspect which is facing may be sufficient. In the case of such an embodiment, not only light emitted from the first organic EL element but also light emitted from the second organic EL element can be taken out from the first substrate side, and from the second substrate side. In addition to the light emission from the second organic EL element, the light emission from the first organic EL element can be taken out, so that the resolution of the organic EL panel obtained on both sides can be doubled, and a sense of depth There is an advantage that can be expressed. Further, as compared with the case where the resolution is increased by using only the first organic EL element, since the interval between the arrangements of the individual organic EL elements can be widened, there is also an advantage that manufacture is facilitated.
Moreover, the method of planar arrangement of the plurality of first organic EL elements and the second organic EL elements is not particularly limited. 6 and 7 are partially enlarged schematic plan views illustrating the planar arrangement of a plurality of first organic EL elements and second organic EL elements. For example, as shown in FIG. 6, it may be arranged in a stripe shape, or may be arranged in a grid pattern as shown in FIG.

(1) First electrode layer and second electrode layer The first electrode layer and the second electrode layer formed on the substrate are formed by, for example, a method such as vacuum sputtering or vacuum deposition, or by applying a coating solution. The manufacturing method is not particularly limited.

In the present invention, the first electrode layer disposed on the substrate side is required to be transparent because light is derived from the substrate side.
Any of the first electrode layer and the second electrode layer may be an anode, but usually the first electrode layer is formed as an anode and the second electrode layer is formed as a cathode. Examples of the material for the electrode layer when formed as such an anode include metals having a large work function such as indium tin oxide (ITO), indium oxide, and gold, polyaniline, polyacetylene, polyalkylthiophene derivatives, and polysilane derivatives. And the like, and the like. On the other hand, materials used when the electrode layer is formed as a cathode include magnesium alloys such as MgAg, aluminum alloys such as AlLi, AlCa, and AlMg, alkaline metals such as Li and Ca, and alkaline earth metals. And metals having a small work function such as alloys of these alkali metals and alkaline earth metals.

(2) Organic EL layer In the present invention, an organic EL layer is formed between the first electrode layer and the second electrode layer as described above. Since the film thickness of this organic EL layer is usually about 1 nm to 2 μm, preferably about 10 nm to 200 nm, it is used at a predetermined pressure in order to place the organic EL layers on both sides back to back in impact during use or transportation. Scratches and cracks are likely to occur when they are bonded together. However, in this invention, since it has the structure which covers an organic EL element with the said filling layer which has high intensity | strength, high elasticity, and a softness | flexibility, damage to such an organic EL element can be suppressed. .

  The organic EL layer referred to in the present invention is formed from one or a plurality of organic layers including a light emitting layer. That is, the organic EL layer is a layer including at least a light emitting layer, and the layer configuration is a layer having one or more organic layers. Usually, when an organic EL layer is formed by a wet method by coating, it is often difficult to stack a large number of layers in relation to a solvent, so that it is often formed of one or two organic layers. However, it is possible to further increase the number of layers by devising organic materials or combining vacuum deposition methods.

  Examples of the organic layer formed in the organic EL layer other than the light emitting layer include a carrier injection layer such as a hole injection layer and an electron injection layer. Furthermore, examples of other organic layers include carrier transport layers such as a hole transport layer and an electron transport layer. Usually, these layers provide a carrier transport function to the carrier injection layer, thereby providing a carrier transport layer. In many cases, they are formed integrally. In addition, examples of the organic layer formed in the EL layer include a layer such as a carrier block layer for suppressing penetration of holes or electrons and improving recombination efficiency.

Examples of the light emitting material used in the light emitting layer essential for the organic EL layer in the present invention include the following.
Examples of dye-based light emitting materials include cyclopentadiene derivatives, tetraphenylbutadiene derivatives, triphenylamine derivatives, oxadiazole derivatives, pyrazoloquinoline derivatives, distyrylbenzene derivatives, distyrylarylene derivatives, silole derivatives, thiophene ring compounds, pyridine rings Examples thereof include compounds, perinone derivatives, perylene derivatives, oligothiophene derivatives, trifumanylamine derivatives, oxadiazole dimers, and pyrazoline dimers.

  Examples of the metal complex light emitting material include aluminum quinolinol complex, benzoquinolinol beryllium complex, benzoxazole zinc complex, benzothiazole zinc complex, azomethylzinc complex, porphyrin zinc complex, europium complex, etc. Or a metal complex having a rare earth metal such as Tb, Eu, or Dy and having a oxadiazole, thiadiazole, phenylpyridine, phenylbenzimidazole, quinoline structure, or the like as a ligand.

  Furthermore, the polymer-based light emitting materials include polyparaphenylene vinylene derivatives, polythiophene derivatives, polyparaphenylene derivatives, polysilane derivatives, polyacetylene derivatives, polyvinylcarbazole, polyfluorenone derivatives, polyfluorene derivatives, polyquinoxaline derivatives, and their co-polymers. A coalescence etc. can be mentioned.

  A dopant may be added to the light emitting layer for the purpose of improving the light emission efficiency and changing the light emission wavelength. Examples of such doping agents include perylene derivatives, coumarin derivatives, rubrene derivatives, quinacridone derivatives, squalium derivatives, porphyrin derivatives, styryl dyes, tetracene derivatives, pyrazoline derivatives, decacyclene, phenoxazone, quinoxaline derivatives, carbazole derivatives, fluorene derivatives, etc. Can be mentioned.

  As the material for forming the hole injection layer, in addition to the compounds exemplified as the light emitting material of the light emitting layer, oxidation of phenylamine, starburst amine, phthalocyanine, vanadium oxide, molybdenum oxide, ruthenium oxide, aluminum oxide, etc. And derivatives of amorphous carbon, polyaniline, polythiophene and the like.

  Further, as the material for forming the electron injection layer, in addition to the compounds exemplified as the light emitting material of the light emitting layer, aluminum, lithium fluoride, strontium, magnesium oxide, magnesium fluoride, strontium fluoride, calcium fluoride, barium fluoride Alkali metals such as aluminum oxide, strontium oxide, calcium, sodium polymethylmethacrylate polystyrene sulfonate, lithium, cesium, cesium fluoride, etc., alkali metal halides, alkali metal organic complexes, etc. it can.

(3) Barrier layer In this invention, you may provide a barrier layer so that the surface which is not in contact with the base | substrate of an organic EL element, ie, the upper surface of an organic EL element, and the circumference | surroundings (side surface) whole may be covered. In such a case, the effect of suppressing deterioration of the organic EL element is further improved. Such a barrier layer is preferably a film formed by a plasma CVD method in consideration of an influence on an element at the time of formation. In particular, SiN, SiO _X N _Y (X, Y formed by a plasma CVD method is preferable. = 0 to 2). In addition, in this invention, since the structure which improved the deterioration suppression of the above organic EL elements is employ | adopted, there also exists an effect that such a barrier layer does not need to be formed.

(4) Others In the organic EL device of the present invention, in addition to the above-described members, various members such as a light extraction improving sheet, a color filter, an antireflection sheet, a circular deflection sheet, a heat radiating sheet, and the like may be used as necessary. You may make it form.

II. Manufacturing method of double-sided light emitting organic EL panel The method of manufacturing a double-sided light emitting organic electroluminescence panel according to the present invention comprises the steps of preparing a first organic electroluminescent element disposed on a first substrate,
Providing a second organic electroluminescent element disposed on the second substrate;
The second organic electroluminescence element on the second substrate is exposed so that the peripheral portion of the surface on which the element of the second substrate is disposed is exposed in the filling layer containing the thermoplastic rubber component as a main component. Forming a laminated body a by laminating on and around the substrate;
The first organic electroluminescence is arranged on the first substrate so that the filling layer of the laminated body a is disposed on and around the first organic electroluminescence element. Laminating on the element to form a laminate b;
A curable resin composition is applied around the filling layer so as to seal between the first substrate and the second substrate in the laminate b, and a curing reaction is performed to form a sealing layer. Process.

  The manufacturing method of the organic EL panel according to the present invention can easily obtain a double-sided light emitting organic EL panel in which the deterioration of the organic EL element is suppressed by having the above-described steps. In addition, the organic EL panel manufacturing method according to the present invention includes a laminate in which a filling layer is laminated in advance on one EL element, and the other EL element is laminated. It is possible to obtain an organic EL panel in which the clearance between the two substrates and between the organic EL elements is uniformly held by the filling layer. Furthermore, since the manufacturing method of the organic EL panel according to the present invention includes the steps as described above, the organic EL panel is not exposed to a component that deteriorates elements such as a curing component and a solvent component in the sealing layer material. There is an effect that the element is not deteriorated and an effect that the sealing substrate is not necessary and the thickness can be reduced by the thickness of the sealing substrate.

  Such a method for producing an organic EL panel of the present invention will be specifically described with reference to the drawings. FIG. 3A to FIG. 3H are process charts showing an example of a method for producing an organic EL panel according to the present invention. As shown in FIG. 3A, first, the first organic EL element 2 disposed on the first substrate 1 is prepared. Also, as shown in FIG. 3B, a second organic EL element 4 arranged on the second substrate 3 is prepared. Next, as shown in FIG. 3 (C), the filling layer 5 containing the specific rubber component is first exposed so that the peripheral edge 10 of the surface on which the elements of the second base 3 are arranged is exposed. A stacked body a (11) is formed by stacking on and around the second organic EL element 4 on the second substrate 3. 3C is a schematic cross-sectional view, while FIG. 3D is a schematic plan view of FIG. 3C viewed from the side where the filling layer 5 is laminated.

  Next, as illustrated in FIG. 3E, the stacked body a (11) is placed so that the filling layer 5 of the stacked body a (11) is disposed on and around the first organic EL element 2. The laminate b (12) is formed by laminating on the first organic EL element 2 arranged on the first substrate 1. Next, as shown in FIG. 3 (F), a curable resin is provided around the filling layer 5 so as to seal between the first base 1 and the second base 3 in the laminate b (12). Composition 13 is applied. Next, as shown in FIG. 3 (G), light and / or heat 14 is applied to the curable resin composition 13 to perform a curing reaction to form the sealing layer 6, and the book as shown in FIG. 3 (H). A double-sided organic EL panel according to the invention can be obtained.

(1) Step of preparing an organic electroluminescence element arranged on a substrate The step of preparing an organic electroluminescence element arranged on a substrate is not particularly limited, and corresponds to the configuration of the organic EL element as appropriate. Various production methods known in the technical field can be used. The area of the surface of the substrate is larger than the area of the surface of the organic EL element so that the periphery of the organic EL element can be sealed with a filling layer or a sealing layer.

(2) Step of forming laminate a The filling layer containing a thermoplastic rubber component as a main component is formed on the second substrate so that the peripheral portion of the surface on which the elements of the second substrate are disposed is exposed. A laminated body a is formed by laminating on and around the second organic EL element. About the material used for a filling layer, since the thing similar to what was demonstrated with the said organic electroluminescent panel can be used, description here is abbreviate | omitted.

When the filling layer is laminated on and around the second organic EL element, the filling layer may be laminated directly on the second organic EL element, or it may be formed after the filling layer is formed on the release treatment film. The filled layer may be transferred and laminated on the second organic EL element. After forming the filling layer on the release film, transferring the formed filling layer onto the second organic EL element and laminating makes it difficult to damage the organic EL element, and the thickness of the filling layer is constant. It is easy to keep the clearance between the first and second substrates constant,
Furthermore, a laminator can be used as a bonding apparatus, which is preferable from the viewpoint of workability.

  When laminating the filling layer on and around the second organic EL element on the second substrate, a sealing layer with at least a sealable thickness is filled in order to provide a sealing layer later for sealing. The peripheral edge of the surface of the second substrate is exposed by adjusting as appropriate within a range that can be provided in contact with the second substrate around the layer (see FIGS. 3C and 3D). . Accordingly, the surface of the filling layer is appropriately smaller than the surface of the substrate. On the other hand, the filling layer is laminated on the organic EL element so as to be disposed on and around the first and second organic EL elements. Therefore, the surface of the filling layer has an area that is appropriately larger than the surfaces of the first and second organic EL elements to such an extent that the surface can be disposed on and around the first and second organic EL elements. To be.

  The size of the peripheral edge portion to be exposed of the substrate may be appropriately adjusted within a range in which at least a sealing layer having a sealable thickness can be provided in contact with the substrate around the filling layer. It is not particularly limited because it differs depending on the case. The peripheral edge of the base exposed can be provided, for example, by leaving about 1 to 30 mm from the end of the base over the entire periphery.

The filling layer is prepared by dissolving a material used for the filling layer in a solvent to prepare a coating liquid for forming a filling layer, and using the coating liquid for forming the filling layer, for example, coating on a release-treated film, and then the solvent. It can also be obtained by drying. However, in the present invention, the filling layer is preferably formed on the release-treated film by melting the material used for the filling layer without using a solvent. This is because, in the case of directly contacting the organic EL element, it is preferable to eliminate the influence of the residual solvent as much as possible from the viewpoint of suppressing deterioration of the element.
Moreover, before the laminated body a prepared by this invention is laminated | stacked on an organic EL element, it is preferable that the filling layer surface by the side laminated | stacked on an EL element is also protected by the peeling process film.

  For example, die coating, roll coating, reverse coating, gravure coating, knife coating, blade coating, rod coating, curtain coating, slide coating, spin coating, screen printing, offset printing, flexography Printing etc. are mentioned. Moreover, melt extrusion coating etc. are mentioned as a method of melting and forming a filled layer. In addition, after forming the filling layer on the release-treated film, as a means for transferring and laminating the formed filling layer on the second organic EL element, laminating is performed by using a laminator while appropriately heating. Method, press method, autoclave method and the like. The surface on the second organic EL element side and the surface on the filling layer side on the release treatment film are opposed to each other so that the filling layer completely covers the second organic EL element. Since the filling layer mainly composed of the rubber component and the tackifying resin as described above is a thermoplastic resin, it can be wet and spread on the EL element and the substrate without heating by heating at about 50 to 150 ° C. On the other hand, when it is returned to room temperature, it exhibits high strength, high elasticity, and flexibility.

  The filling layer can be formed in various thicknesses so as to appropriately cover the organic EL element, but is usually in the range of 1 to 200 μm, preferably in the range of 3 to 100 μm, more preferably. , In the range of 5 to 50 μm.

  As shown in FIG. 2, when the getter layer 7 is provided as a layer separate from the filling layer 5, the method of providing the getter layer is not particularly limited. For example, a method in which a laminate a is prepared by using a layer in which a getter layer is provided between two filler layers in advance as a single laminated layer. In this case, the getter layer can be formed using a conventionally known method in accordance with a selected material.

  In addition, when preparing the laminate a, it is preferably performed in an environment where the oxygen concentration and the water concentration are low, for example, performed under conditions such as a nitrogen atmosphere, an oxygen concentration of 1 ppm, a water concentration of 10 ppm or less, It is preferable from the viewpoint of suppressing deterioration of the organic EL element due to moisture and oxygen.

(3) Step of forming the laminated body b The laminated body a is arranged on the first base so that the filling layer of the laminated body a is arranged on and around the first organic EL element. A stacked body b is formed on the first organic EL element thus formed (see FIG. 3E).
Before the laminate a is laminated on the first organic EL element, moisture and oxygen adsorbed on the laminate a during storage are removed by, for example, CaO, CaCO ₃ , BaO, silica gel, molecular sieve, or the like. Is preferable from the viewpoint of suppressing deterioration of the organic EL element.

  Lamination is performed so that the first organic EL element side surface disposed on the first substrate faces the filling layer side surface of the laminate a so that the filling layer completely covers the first organic EL element. To do. Examples of the laminating method include a laminating method in which a laminator is used while appropriately heating, a pressing method, an autoclave method, and the like.

  Further, as shown in FIG. 5 described above, a plurality of first organic electroluminescence elements arranged in a plane with a predetermined interval on the first substrate and a predetermined interval on the second substrate. A plurality of planarly arranged second organic electroluminescence elements, and at least a first non-light emitting portion and a second organic electroluminescence existing between the plurality of first organic electroluminescence elements. The laminated body a so that the element faces and the second non-light-emitting portion existing between the plurality of second organic electroluminescence elements faces the first organic electroluminescence element. May be laminated on the first organic electroluminescence element disposed on the first substrate to form a laminate b.

  Even in the case of forming the laminated body b, it is preferable to carry out in an environment where the oxygen concentration and the water concentration are low. This is preferable from the viewpoint of suppressing deterioration of the element due to moisture and oxygen.

(4) Step of forming a sealing layer First, a curable resin composition is applied around the filling layer so as to seal between the first and second substrates in the laminate b (FIG. 3). (See (F)). A curable resin composition is applied around the filler layer in the gap between the first and second substrates so that the surface of the filler layer is not exposed. By doing in this way, since between the said 1st and 2nd base | substrate in the said laminated body b can be sealed and an organic EL element can be sealed, deterioration of an organic EL element can be suppressed.

As the curable resin composition used for forming the sealing layer, a composition mainly composed of the curable resin described in the sealing layer can be used, and the description thereof is omitted here.
Examples of the method for applying the curable resin composition include a method using a dispenser and a screen printing method.

  Next, in accordance with the curable resin composition used, light irradiation such as ultraviolet rays and electron beams and / or heating is performed to perform a curing reaction (see FIG. 3G) to form a sealing layer ( (See FIG. 3H). When performing light irradiation, it is preferable to irradiate only the part which apply | coated the photocurable resin composition from the point of deterioration suppression of an organic EL element.

  As mentioned above, although each process was demonstrated about the manufacturing method of the organic electroluminescent panel which concerns on this invention, the organic electroluminescent panel which concerns on the said invention is not limited to the manufacturing method of the organic electroluminescent panel which concerns on the said invention, It can manufacture. it can. For example, as shown in FIGS. 4 (A) and 4 (B), a laminate a (11) in which a sealing layer 6 is previously laminated on the base 3 together with the filling layer 5 in a frame shape around the filling layer. The sealing layer may be formed by laminating on the organic EL element on the other substrate. In this case, a photocurable resin composition having a relatively high viscosity is preferably used for the sealing layer. For such a sealing layer, a photocurable resin having a relatively high viscosity may be selected and used, a delayed curable photocurable resin may be used, or a curable type so as to increase the viscosity. You may add and use additives, such as a filler, suitably to resin.

  The present invention is not limited to the above embodiment. The above-described embodiment is an exemplification, and the present invention has any configuration that has substantially the same configuration as the technical idea described in the claims of the present invention and that exhibits the same effects. Are included in the technical scope.

<Example 1>
1. Production of Organic EL Element Two organic EL elements arranged on the substrate were prepared as follows.
First, a glass substrate with an ITO film (manufactured by Sanyo Vacuum Industry Co., Ltd., ITO film thickness: 150 nm, sheet resistance: 14 Ω / □, glass thickness 0.7 mm, outer dimensions 150 mm × 150 mm) was prepared. The ITO film was patterned by a photolithography method to form an ITO electrode pattern.

  The surface of the obtained substrate with the ITO electrode pattern was wet-cleaned, and an insulating layer was formed by photolithography. The number of pixels was 40 × 40, the openings were 2.0 mm □, the pixel pitch was 2.5 mm, and the insulating layer height was 1.5 μm. Thereafter, a cathode separator having a height of 4 μm was formed between the pixel pitches in the cathode direction by photolithography.

A surface treatment was performed on the substrate with an atmospheric pressure plasma apparatus, and then a hole injection layer with a thickness of 60 nm and an organic light emitting layer with a thickness of 90 nm were formed by gravure printing.
As the hole injection material, poly 3,4-ethylenedioxythiophene / polystyrene sulfonate aqueous dispersion (PEDOT / PSS = 1: 20, trade name: CLEVIOS P CH8000, HCStarck) is used and formed by gravure printing Then, drying was performed in the atmosphere at 120 ° C. for 30 minutes. Also, as the organic light emitting material, a polyfluorene derivative-based green light emitting material (weight average molecular weight 300,000) is formed by gravure printing, followed by drying at 180 ° C. for 1 hour at an oxygen concentration of 1 ppm or less in a nitrogen atmosphere. It was.

Thereafter, a Ca layer (electron injection layer) having a thickness of 10 nm and an Al electrode having a thickness of 300 nm were stacked by vacuum deposition. The pressure during vacuum deposition was 2 × 10 ⁻⁷ torr. The deposition rate was about 1.0 Å / s for Ca and about 5 Å / s for aluminum.

2. Production of laminate a: 100 parts by weight of a styrene-isoprene-styrene resin (manufactured by JSR, SIS 5200, styrene content 15 mol%, diblock content 20% by weight) as a rubber component of the packed layer, and an alicyclic as a tackifier resin 100 parts by weight of a saturated hydrocarbon resin (Arakawa Chemical Industries, Alcon P-100, softening point 100 ° C.) was used. The rubber component was heated and dissolved at 150 to 200 ° C. for 60 minutes, and the tackifying resin was added to the dissolved rubber component. The rubber component and the tackifier resin were mixed and stirred until they were in a uniform state to obtain a resin mixture for forming a packed bed.

Using a spreader, apply the resin mixture for forming a filling layer obtained above to a peeled surface of a 38 μm-thick release treatment polyester film (Purex, manufactured by Teijin DuPont Films Co., Ltd.) so as to be 50 g / m ^2. did. The packed layer side was further laminated with a peeled surface of a 38 μm release treated polyester film (Fujimori Kogyo Co., Ltd., film binder) to prepare a packed layer sheet having a uniform thickness. The thickness of the obtained packed bed was 50 μm.

About the obtained packed bed, when the water vapor transmission rate was measured using a water vapor transmission rate measuring device (MOCON water vapor transmission rate measuring device PERMATRAN-W 3/61 manufactured by MOCON) in an atmosphere of 60 ° C. and 90% RH, 10 g / m ² / day.
Moreover, about the obtained filling layer, it was 23 N / 25mm when the 180 degree peeling test was done with respect to the stainless steel plate according to JIS Z 0237, and the adhesive force was measured.

  The packed bed sheet formed as above was cut into an outer dimension of 115 mm × 115 mm. The release-treated polyester film on one side of the filling layer sheet is peeled off, and the filling layer sheet is filled using a laminator at the center of the substrate on which one of the two organic EL elements obtained above is disposed. The surface on the layer side was pasted (nitrogen atmosphere oxygen concentration 1 ppm or less, roll temperature 70 ° C.). In this way, the layered product a was formed by laminating the filling layer on and around the organic electroluminescence element on the base so that the peripheral portion of the surface on which the base element was disposed was exposed.

3. Production of double-sided light emitting organic EL panel The double-sided light emitting organic EL panel of the present invention was produced as follows.
The other release-treated polyester film on the packed layer of the laminate a obtained above was peeled off to remove moisture adsorbed on the packed layer. Of the two organic EL elements obtained above, the element-side surface of the other organic EL element is opposed to the surface of the stacked body a on the filling layer side, and the filling layer is on and around the other EL element. Also, a laminator was used so as to completely cover the EL pixel portion. (Nitrogen atmosphere oxygen concentration 1ppm or less, roll temperature 70 ℃)

  A thermosetting epoxy resin (manufactured by ThreeBond Co., two-pack epoxy resin; 20X-325) is applied to the gap formed between the two substrates (the outer periphery of the filling layer) using a dispenser, and 80 C. for 1 hour to form a sealing layer.

The obtained double-sided light-emitting organic EL panel of Example 1 was stored in the atmosphere at room temperature for 10 days, and then a 12 V DC voltage was applied to observe the light emitting part. No dark spots were observed.
It was estimated that the gas barrier properties from moisture and oxygen were improved and the organic EL element was not deteriorated by impurities generated from the sealant.
The clearance between the organic EL elements was uniformly maintained by the filling layer.

<Example 2>
Instead of using a glass substrate as the base of the two organic EL elements, a sealing gas barrier film (PEN base material (thickness 200 μm, manufactured by Teijin DuPont, Teonex Q65F) is used as a base, and SiOxNy (x, y = 0 to 2 ) Inorganic layer and organic layer hybridized in the same manner as in Example 1 except that a water vapor transmission rate of 1 × 10 ⁻³ g / m ² / day or less) was used. Manufactured.

The obtained double-sided light emitting organic EL panel of Example 2 was stored in the atmosphere at room temperature for 10 days, and then a 12 V DC voltage was applied to observe the light emitting part. As a result, no dark spots were observed.
It was estimated that the gas barrier properties from moisture and oxygen were improved and the organic EL element was not deteriorated by impurities generated from the sealant.
The clearance between the organic EL elements was uniformly maintained by the filling layer. Further, it was confirmed that the organic EL panel sample was flexible so that its appearance and performance did not change even after a test in which the sample was wound around a 60 mmφ rod.

<Example 3>
When forming the sealing layer, a UV curable adhesive (WORLD ROCK 8723L2 manufactured by Kyoritsu Chemical Industry Co., Ltd.) is used in the gap formed between the two substrates (the outer periphery of the filling layer) using a dispenser. A double-sided light emitting organic EL panel was produced in the same manner as in Example 1 except that only the coated part was irradiated with ultraviolet rays under conditions of 6 J / cm ² or more and cured to form a sealing layer. .

The obtained double-sided issue type organic EL panel of Example 3 was stored in the atmosphere at room temperature for 10 days, and then a 12 V DC voltage was applied to observe the light emitting part, and no dark spots were observed.
It was estimated that the gas barrier properties from moisture and oxygen were improved and the organic EL element was not deteriorated by impurities generated from the sealant.
The clearance between the organic EL elements was uniformly maintained by the filling layer.

<Example 4>
Instead of using a glass substrate as the base of the organic EL element, a sealing gas barrier film (PEN base material (thickness: 200 μm, manufactured by Teijin DuPont, Teonex Q65F) is used as a base, and SiOxNy (x, y = 0 to 2) A double-sided organic EL panel was manufactured in the same manner as in Example 3 except that a hybrid of an inorganic layer and an organic layer (water vapor transmission rate of 1 × 10 ⁻³ g / m ² / day or less) was used. .

The obtained organic EL panel of Example 4 was stored in the atmosphere at room temperature for 10 days, and then a direct current voltage of 12 V was applied to observe the light emitting part. No occurrence of dark spots was observed.
It was estimated that the gas barrier properties from moisture and oxygen were improved and the organic EL element was not deteriorated by impurities generated from the sealant.
The clearance between the organic EL elements was uniformly maintained by the filling layer. Further, it was confirmed that the organic EL panel sample was flexible so that its appearance and performance did not change even after a test in which the sample was wound around a 60 mmφ rod.

<Example 5>
An organic EL panel was produced in the same manner as in Example 1 except that the filling layer was formed using the resin mixture for forming a filling layer as described below.
100 parts by weight of Kuraray Septon 2063 (styrene content 13 mol%, JISA rubber hardness 36 °) as styrene-ethylene-propylene-styrene copolymer rubber (SEPS), and alicyclic saturated hydrocarbon as tackifying resin 100 parts by weight of a resin (Arakawa Chemical Industries, Alcon P-100, softening point 100 ° C.) was used. The rubber component was heated and dissolved at 150 to 200 ° C. for 60 minutes, and the tackifying resin was added to the dissolved rubber component. The rubber component and the tackifier resin were mixed and stirred until they were in a uniform state to obtain a resin mixture for forming a packed bed.

  The obtained organic EL panel of Example 5 was stored in the atmosphere at room temperature for 10 days, and then a direct current voltage of 12 V was applied to observe the light emitting part. No occurrence of dark spots was observed.

<Comparative Example 1>
In Example 1, a double-sided light emitting organic EL panel was produced in the same manner as in Example 1 except that the sealing layer was not formed. After storing in the atmosphere at room temperature for 6 days, a 12 V DC voltage was applied and the light emitting part was observed. As a result, dark spots were observed. It was estimated that the deterioration of the organic EL element was rapid because the gas barrier property against moisture and oxygen was not sufficient in the side surface direction of the organic EL element.

It is sectional drawing which shows an example of the organic electroluminescent panel of this invention typically. It is sectional drawing which shows typically another example of the organic electroluminescent panel of this invention. FIG. 3A to FIG. 3D are process diagrams showing an example of a method for producing an organic EL panel of the present invention. FIG. 3E to FIG. 3H are process diagrams showing an example of a method for manufacturing an organic EL panel according to the present invention. FIG. 4 (A) is a cross-sectional view schematically showing an example of a laminate used for manufacturing the organic EL panel of the present invention, and FIG. 4 (B) is a schematic plan view thereof. It is the typical expanded sectional view which illustrates the method of arrangement | positioning of the organic EL element in the organic EL panel of this invention. FIG. 3 is a partially enlarged schematic plan view illustrating a planar arrangement of a plurality of organic EL elements in the organic EL panel of the present invention. FIG. 3 is a partially enlarged schematic plan view illustrating a planar arrangement of a plurality of organic EL elements in the organic EL panel of the present invention.

Explanation of symbols

DESCRIPTION OF SYMBOLS 1 1st base | substrate 2 1st organic EL element 3 2nd base | substrate 4 2nd organic EL element 5 Filling layer 6 Sealing layer 7 Getter layer 10 Peripheral part 11 Laminated body a
12 Laminated body b
13 curable resin composition 14 light and / or heat 15 first non-light emitting portion 16 second non-light emitting portion

Claims (21)

A first substrate, a first organic electroluminescence element disposed on the substrate, a second substrate, and a second organic electroluminescence element disposed on the substrate are first and second. In the double-sided light emission type electroluminescence panel having the organic electroluminescence elements of
A filling layer disposed between and around the first and second organic electroluminescence elements, and a seal disposed in a frame shape around the filling layer in contact with the first substrate and the second substrate. A stop layer,
The double-sided light emitting organic electroluminescence panel, wherein the filling layer contains a thermoplastic rubber component as a main component, and the sealing layer contains a curable resin as a main component.   The packed bed is composed of ABA type styrene block copolymer rubber and / or hydride thereof 50 to 100% by weight, and AB type styrene block copolymer rubber and / or hydride 0 to 50 thereof. 2. The organic electroluminescence panel according to claim 1, comprising, as a main component, a rubber component composed of wt% and 50 parts by weight or more of a tackifier resin with respect to 100 parts by weight of the rubber component.   The packed layer is made of styrene-isoprene-styrene block copolymer rubber, styrene-butadiene-styrene copolymer rubber, styrene-ethylene-butylene-styrene copolymer rubber, and styrene-ethylene-propylene-styrene copolymer rubber. The organic electroluminescence panel according to claim 1 or 2, comprising at least one selected from the group consisting of:   The organic electroluminescence panel according to claim 2 or 3, wherein the A-B-A type styrene block copolymer rubber or the hydride thereof in the packed layer is 10 to 40 mol%.   The organic electroluminescence panel according to claim 1, wherein the filling layer does not contain a curing agent.   The organic electroluminescence according to any one of claims 2 to 5, wherein the tackifying resin in the packed layer is at least one selected from the group consisting of hydrogenated petroleum resins, rosin resins, and terpene resins. panel.   The organic electroluminescent panel according to claim 1, wherein the filling layer contains a getter agent.   Furthermore, the organic electroluminescent panel in any one of Claims 1 thru | or 7 containing a getter layer.   The organic electroluminescence panel according to claim 1, wherein the sealing layer contains an epoxy resin as a main component.   The organic electroluminescence panel according to claim 1, wherein the first substrate and / or the second substrate have flexibility.   The organic electroluminescence panel according to claim 1, further comprising a barrier layer between the organic electroluminescence element and the filling layer.   A plurality of first organic electroluminescence elements arranged in a plane with a predetermined interval on the first substrate, and a plurality of planes arranged in a plane with a predetermined interval on the second substrate. Two organic electroluminescent elements, the first non-light emitting portion and the second organic electroluminescent element existing between the plurality of first organic electroluminescent elements are opposed to each other, and the plurality The organic electroluminescence according to any one of claims 1 to 11, wherein the second non-light-emitting portion existing between the second organic electroluminescence elements is opposed to the first organic electroluminescence element. panel. Preparing a first organic electroluminescent element disposed on the first substrate;
Providing a second organic electroluminescent element disposed on the second substrate;
The second organic electroluminescence element on the second substrate is exposed so that the peripheral portion of the surface on which the element of the second substrate is disposed is exposed in the filling layer containing the thermoplastic rubber component as a main component. Forming a laminated body a by laminating on and around the substrate;
The first organic electroluminescence is arranged on the first substrate so that the filling layer of the laminated body a is disposed on and around the first organic electroluminescence element. Laminating on the element to form a laminate b;
A curable resin composition is applied around the filling layer so as to seal between the first substrate and the second substrate in the laminate b, and a curing reaction is performed to form a sealing layer. A method for producing a double-sided light emitting organic electroluminescence panel, comprising: a step.   The packed bed is composed of ABA type styrene block copolymer rubber and / or hydride thereof 50 to 100% by weight, and AB type styrene block copolymer rubber and / or hydride 0 to 50 thereof. The manufacturing method of the organic electroluminescent panel of Claim 13 which contains the rubber component which consists of weight%, and 50 weight part or more tackifying resin with respect to 100 weight part of said rubber components as a main component.   The packed layer is made of styrene-isoprene-styrene block copolymer rubber, styrene-butadiene-styrene copolymer rubber, styrene-ethylene-butylene-styrene copolymer rubber, and styrene-ethylene-propylene-styrene copolymer rubber. The manufacturing method of the organic electroluminescent panel of Claim 13 or 14 containing 1 or more types selected from the group which consists of.   The manufacturing method of the organic electroluminescent panel of Claim 14 or 15 whose styrene component in the ABA type styrene block copolymer rubber or its hydride in the said filling layer is 10-40 mol%.   The organic electroluminescence panel according to any one of claims 13 to 16, wherein in the step of forming the laminate a, the filling layer is melted without using a solvent and laminated on the second substrate. Manufacturing method.   The method for producing an organic electroluminescence panel according to claim 13, wherein the filling layer does not contain a curing agent.   The organic electroluminescence according to any one of claims 14 to 18, wherein the tackifying resin in the packed layer is at least one selected from the group consisting of hydrogenated petroleum resins, rosin resins, and terpene resins. Panel manufacturing method.   The method for manufacturing an organic electroluminescence panel according to claim 13, wherein the sealing layer contains an epoxy resin as a main component. A step of preparing a plurality of first organic electroluminescent elements arranged in a plane on the first substrate at a predetermined interval; and a step of arranging a plurality of planes on the second substrate at a predetermined interval. Preparing a second organic electroluminescence device;
The first non-light-emitting portion and the second organic electroluminescence element that are present between the plurality of first organic electroluminescence elements are opposed to each other, and the plurality of second organic electroluminescence elements are between each other. On the first organic electroluminescent element disposed on the first substrate so that the second non-light emitting portion existing between the first organic electroluminescent element and the first organic electroluminescent element are opposed to each other. The manufacturing method of the organic electroluminescent panel in any one of Claims 13 thru | or 20 which has the process of laminating | stacking on and forming the laminated body b.

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