阅读说明：本技术 有机电子器件的制造方法 (Method for manufacturing organic electronic device ) 是由 下河原匡哉 森岛进一 黑木宏芳 藤本英志 中静勇太 于 2018-12-06 设计创作，主要内容包括：一实施方式的有机电子器件的制造方法包括：器件基材形成工序,形成在基板上依次设置有第一电极、包含有机层的器件功能部、以及第二电极的器件基材；脱水工序(S22),一边输送在密封构件上经由粘接层而层叠有保护膜的带保护膜的密封构件(10)一边进行加热脱水,该密封构件具有密封基材、层叠于密封基材的一面的粘接层、以及层叠于密封基材的另一面的树脂层；以及密封构件贴合工序,从经过了脱水工序的带保护膜的密封构件剥离保护膜,经由粘接层将密封构件贴合于器件基材,在脱水工序中,被输送的带保护膜的密封构件所接触的辊(R1)的辊表面的温度为树脂层的玻璃化转变温度以上。(The method of manufacturing an organic electronic device of an embodiment includes: a device base material forming step of forming a device base material in which a first electrode, a device functional portion including an organic layer, and a second electrode are provided in this order on a substrate; a dehydration step (S22) in which a protective film-equipped sealing member (10) having a sealing base material, an adhesive layer laminated on one surface of the sealing base material, and a resin layer laminated on the other surface of the sealing base material is heated and dehydrated while being conveyed; and a sealing member bonding step of peeling the protective film from the sealing member with the protective film having undergone the dehydration step, and bonding the sealing member to the device substrate via the adhesive layer, wherein in the dehydration step, the temperature of the roller surface of a roller (R1) with which the sealing member with the protective film is in contact with the roller surface is equal to or higher than the glass transition temperature of the resin layer.)

1. A method of manufacturing an organic electronic device, wherein,

the method of manufacturing an organic electronic device includes:

a device base material forming step of forming a device base material in which a first electrode, a device functional portion including an organic layer, and a second electrode are provided in this order on a substrate;

a dehydration step of heating and dehydrating a protective film-equipped sealing member having a sealing base material, an adhesive layer laminated on one surface of the sealing base material, and a resin layer laminated on the other surface of the sealing base material, while conveying the protective film-equipped sealing member, on which the protective film is laminated via the adhesive layer, by at least one roller; and

a sealing member bonding step of peeling the protective film from the sealing member with the protective film having undergone the dehydration step, and bonding the sealing member to the device substrate via the adhesive layer,

in the dehydration step, the temperature of the roller surface of the roller with which the protective film-attached sealing member is in contact is equal to or higher than the glass transition temperature of the resin layer.

2. The method of manufacturing an organic electronic device according to claim 1,

the method for manufacturing an organic electronic device includes a slow cooling step of slowly cooling the sealing member with the protective film to a temperature lower than the glass transition temperature of the resin layer after the dehydration step.

3. The method of manufacturing an organic electronic device according to claim 2,

in the slow cooling step, the sealing member with the protective film is conveyed by a plurality of rollers,

the temperature of the roll surface of the plurality of rolls in the slow cooling step is set to be gradually reduced from a temperature equal to or higher than the glass transition temperature of the resin layer to a temperature lower than the glass transition temperature of the resin layer from the roll on the upstream side toward the roll on the downstream side.

4. The method of manufacturing an organic electronic device according to any one of claims 1 to 3,

the method for manufacturing an organic electronic device includes a preliminary heating step of heating the sealing member with the protective film to a temperature equal to or higher than the glass transition temperature of the resin layer in stages before the dehydration step.

5. The method of manufacturing an organic electronic device according to claim 4,

in the preheating step, the sealing member with the protective film is conveyed by a plurality of preheating rollers,

the temperature of the roller surfaces of the plurality of preheating rollers in the preheating step is set to be gradually increased from a temperature lower than the glass transition temperature of the resin layer to a temperature equal to or higher than the glass transition temperature of the resin layer from the upstream preheating roller toward the downstream preheating roller.

Technical Field

The present invention relates to a method of manufacturing an organic electronic device.

Background

The organic electronic device includes a device base material in which a first electrode, a device functional portion (including an organic layer), and a second electrode are provided in this order on a substrate, and a sealing member that seals the device functional portion. As a sealing member, for example, a sealing member is known in which a barrier layer and an adhesive layer (resin composition layer) are sequentially laminated on a support made of a resin film as described in patent document 1. Such a sealing member is bonded to the device substrate via an adhesive layer. In the technique described in patent document 1, a protective film (cover film) is provided on the adhesive layer of the sealing member until the sealing member is bonded to the device substrate. Since the sealing member is a member for preventing deterioration due to moisture in the organic layer included in the device functional portion, it is preferable that the sealing member itself is also dehydrated.

Prior art documents

Patent document

Patent document 1: international publication No. 2016/152756

Disclosure of Invention

Problems to be solved by the invention

In patent document 1, a sealing member provided with a protective film, that is, a sealing member with a protective film is heated and dehydrated by infrared rays. When the sealing member with the protective film is heated and dehydrated, the sealing member with the protective film tends to be heated at a temperature equal to or higher than the glass transition temperature of the resin film (resin layer) included in the sealing member. In this case, the molecular orientation of the resin film is locally changed. Therefore, for example, the sealing member with the protective film is brought into contact with the conveying roller, and when the contact portion is quenched, wrinkles are generated and fixed. As a result, since wrinkles are also generated in the sealing member, when the sealing member is bonded to the device substrate, bubbles are mixed in the bonding surface, or wrinkles in the bonding surface may not allow sufficient bonding, and thus desired sealing performance may not be secured.

Accordingly, an object of the present invention is to provide a method for manufacturing an organic electronic device capable of providing an organic electronic device having a desired sealing performance.

Means for solving the problems

A method for manufacturing an organic electronic device according to an aspect of the present invention includes: a device base material forming step of forming a device base material in which a first electrode, a device functional portion including an organic layer, and a second electrode are provided in this order on a substrate; a dehydration step of heating and dehydrating a protective film-equipped sealing member having a sealing base material, an adhesive layer laminated on one surface of the sealing base material, and a resin layer laminated on the other surface of the sealing base material, while conveying the protective film-equipped sealing member, which has a protective film laminated on the sealing member via the adhesive layer, by at least one roller; and a sealing member bonding step of peeling the protective film from the protective film-attached sealing member having undergone the dehydration step, and bonding the sealing member to the device base material via the adhesive layer, wherein in the dehydration step, a temperature of a roller surface of the roller, with which the protective film-attached sealing member is in contact, of the conveyed roller surface is equal to or higher than a glass transition temperature of the resin layer.

In the above manufacturing method, in the dehydration step, the temperature of the roll surface of the roll with which the protective film-attached sealing member is in contact is equal to or higher than the glass transition temperature of the resin layer. Therefore, even if the heated sealing member with the protective film comes into contact with the roller in the dehydration step, the sealing member is not rapidly cooled. As a result, the generation of wrinkles in the sealing member with the protective film in the dehydration step and the fixation thereof can be suppressed.

The method of manufacturing an organic electronic device according to an embodiment may further include a slow cooling step of slowly cooling the sealing member with the protective film to a temperature lower than the glass transition temperature of the resin layer after the dehydration step. This can prevent the occurrence of wrinkles in the sealing member with the protective film after the dehydration step.

In the slow cooling step, the sealing member with the protective film may be conveyed by a plurality of rollers, and the temperature of the roller surface of the plurality of rollers in the slow cooling step may be set to be gradually reduced from a temperature equal to or higher than the glass transition temperature of the resin layer to a temperature lower than the glass transition temperature of the resin layer from the roller on the upstream side toward the roller on the downstream side. In this way, in the slow cooling step, the protective film-attached sealing member is not rapidly cooled by being brought into contact with the plurality of rollers, and therefore wrinkles can be prevented from being generated.

The method of manufacturing an organic electronic device according to one embodiment may further include a preliminary heating step of heating the sealing member with the protective film to a temperature equal to or higher than the glass transition temperature of the resin layer in stages before the dehydration step. In the preheating step, the sealing member of the protective film is conveyed by a plurality of preheating rollers, and the temperature of the roller surfaces of the plurality of preheating rollers in the preheating step may be set to be gradually increased from a temperature lower than the glass transition temperature of the resin layer to a temperature higher than or equal to the glass transition temperature of the resin layer from the upstream preheating roller toward the downstream preheating roller.

Effects of the invention

According to the present invention, a method for manufacturing an organic electronic device can be provided, which can provide an organic electronic device having desired sealing performance.

Drawings

Fig. 1 is a side view of a sealing member with a protective film according to an embodiment.

Fig. 2 is a flowchart showing a method for manufacturing an organic EL device (organic electronic device) using the sealing member with the protective film shown in fig. 1.

Fig. 3 is a cross-sectional view showing an example of the structure of a device substrate included in an organic EL device to be manufactured.

Fig. 4 is a diagram for explaining the preparation process shown in fig. 2.

Fig. 5 is a diagram for explaining a sealing member bonding step in the method for manufacturing an organic EL device (organic electronic device).

Detailed Description

Hereinafter, embodiments of the present invention will be described with reference to the drawings. The same elements are denoted by the same reference numerals, and redundant description is omitted. The dimensional ratios in the drawings do not necessarily correspond to the dimensional ratios illustrated.

Fig. 1 is a side view of a sealing member 10 with a protective film for manufacturing an organic EL device (organic electronic device) of an embodiment. Fig. 1 schematically shows the structure of the sealing member with protective film 10. The sealing member with a protective film 10 includes a sealing member 20 and a protective film 30. The sealing member with protective film 10 may be a tape or a single sheet. Hereinafter, unless otherwise specified, the sealing member 10 with a protective film is in a band shape.

The sealing member 20 is a member for preventing deterioration of an organic layer included in the organic EL device. The sealing member 20 includes a sealing base material 21, an adhesive layer 22, and a resin film (resin layer) 23.

The sealing substrate 21 has a moisture barrier function. Examples of the moisture permeability of the sealing substrate 21 are at a temperature of 40 ℃ and a humidity of 90% RH of 5 × 10 under ambient conditions^-5g/(m²24hr) or less. The water vapor transmission rate can be measured by, for example, the calcium corrosion method. The sealing substrate 21 may have a gas barrier function. Examples of the sealing substrate 21 include a metal foil, a barrier film having a barrier functional layer formed on one surface or both surfaces of a transparent plastic film, a flexible film glass, and a film in which a metal having barrier properties is laminated on a plastic film. Examples of the thickness of the sealing substrate 21 are 10 μm to 300 μm. As the metal foil, a copper foil, an aluminum foil, or a stainless steel foil is preferable from the viewpoint of barrier property. When the sealing substrate 21 is a metal foil, the thickness of the metal foil is preferably as large as possible from the viewpoint of suppressing pinholes, but is preferably 10 μm to 50 μm from the viewpoint of flexibility.

The adhesive layer 22 is laminated on one surface of the sealing substrate 21. The adhesive layer 22 is a layer disposed to adhere at least two adjacent layers to each other. The adhesive layer 22 may have a thickness that allows embedding of a portion of the organic EL device to be sealed by the sealing member 20. Examples of the thickness of the adhesive layer 22 are 5 μm to 100 μm.

Examples of the material of the adhesive layer 22 include a photocurable or thermosetting acrylate resin, a photocurable or thermosetting epoxy resin, and the like. Other generally used resin films that can be welded by impulse heat sealing, for example, heat-weldable films such as ethylene-vinyl acetate copolymer (EVA), polypropylene (PP) film, Polyethylene (PE) film, and polybutadiene film, can be used as the adhesive layer 22. Thermoplastic resins can also be used for the material of the adhesive layer 22. Examples of the thermoplastic resin include olefin elastomers, styrene elastomers, and butadiene elastomers.

The adhesive layer 22 may also contain a moisture absorbent. The moisture absorbent is an agent that absorbs moisture. The moisture absorbent can absorb oxygen and the like in addition to moisture. The moisture absorption rate of the moisture absorbent is preferably 1 wt%/hr or more in an environment of 24 ℃ and 55% RH.

The resin film 23 is laminated on the other surface (the surface opposite to the surface in contact with the adhesive layer 22) of the sealing substrate 21. The resin film 23 can function as a support for the sealing substrate 21. Examples of the material of the resin film 23 include polyethylene terephthalate (PET), Polyimide (PI), and the like.

The protective film 30 is laminated on the surface of the adhesive layer 22 opposite to the surface in contact with the sealing substrate 21. That is, the protective film 30 is laminated on the sealing member 20 via the adhesive layer 22. The protective film 30 is a member for preventing adhesion of dust to the adhesive layer 22 and adhesion of the adhesive layer 22 to a plurality of conveying rollers R described later before the organic EL device is manufactured. The protective film 30 may be a release film that can be peeled from the adhesive layer 22.

Examples of the material of the protective film 30 include polyethylene naphthalate (PEN), PET, PP, PE, PI, cycloolefin polymer, cycloolefin copolymer, and the like. Examples of the thickness of the protective film 30 include 9 μm to 50 μm.

The coating layer may be formed on the surface of the protective film 30 that contacts the adhesive layer 22. Examples of the material of the coating layer include silicone resin-based release agents, fluorine-based release agents, alkyd-based release agents, acrylic release agents, and the like.

Next, an example of a method for manufacturing an organic EL device using the sealing member with protective film 10 shown in fig. 1 will be described. As shown in fig. 2, the method of manufacturing an organic EL device includes: a device substrate forming step S10, a preparation step S20 of the sealing member with protective film 10, and a sealing member bonding step S30. Unless otherwise specified, the description will be made in correspondence with the case where the organic EL device to be manufactured is of a bottom emission type, but the organic EL device may be of a top emission type.

[ device substrate Forming Process ]

In the device substrate forming step S10, as shown in fig. 3, the anode (first electrode) 42, the organic EL section (device function section including organic layers) 43, and the cathode (second electrode) 44 are sequentially stacked on the substrate 41 to form the device substrate 40. The device substrate 40 will be explained.

[ base plate ]

The substrate 41 has a light-transmitting property with respect to light (including visible light having a wavelength of 400nm to 800 nm) emitted from the organic EL device to be manufactured. In the present embodiment, the substrate 41 used for manufacturing the organic EL device has a belt shape. Examples of the thickness of the substrate 41 are 30 μm to 700 μm.

The substrate 41 is preferably a flexible substrate. The flexibility means a property that the substrate can be flexed without shearing or breaking even if a predetermined force is applied to the substrate. Examples of the substrate 41 are a plastic film or a polymer film. The substrate 41 may further have a barrier layer having a moisture barrier function. The barrier layer may have a function of blocking a gas (e.g., oxygen) in addition to a function of blocking moisture.

[ Anode ]

The anode 42 is disposed on the substrate 41. An electrode exhibiting light transmittance is used for the anode 42. As the electrode exhibiting light transmittance, a thin film containing a metal oxide, a metal sulfide, a metal, or the like having high electrical conductivity can be used, and a thin film having high light transmittance is preferably used. The anode 42 may have a network structure formed of an electrical conductor (e.g., metal). The thickness of the anode 42 may be determined in consideration of light transmittance, electrical conductivity, and the like. The thickness of the anode 42 is usually 10nm to 10 μm, preferably 20nm to 1 μm, and more preferably 50nm to 500 nm.

Examples of the material of the anode 42 include Indium Oxide, Zinc Oxide, tin Oxide, Indium Tin Oxide (ITO), Indium Zinc Oxide (IZO), gold, platinum, silver, and copper, and among them, ITO, IZO, and tin Oxide are preferable. Anode 42 can be formed as a thin film comprising the materials illustrated. As the material of the anode 42, organic substances such as polyaniline and its derivatives, polythiophene and its derivatives, and the like can be used. In this case, the anode 42 may be formed as a transparent conductive film.

The anode 42 can be formed by a dry film formation method, an electroplating method, a coating method, or the like. Examples of the dry film formation method include a vacuum deposition method, a sputtering method, an ion plating method, and a CVD method. Examples of the coating method include an ink jet printing method, a slit coating method, a micro gravure coating method, a bar coating method, a roll coating method, a wire bar coating method, a spray coating method, a screen printing method, a flexo printing method, an offset printing method, a nozzle printing method, and the like, and among them, the ink jet printing method is preferable.

[ organic EL part ]

The organic EL section 43 is a functional section that contributes to light emission of the organic EL device, such as movement of electric charges and recombination of electric charges, in accordance with voltages applied to the anode 42 and the cathode 44. The organic EL section 43 has organic layers such as a light-emitting layer.

The light-emitting layer is a functional layer having a function of emitting light (including visible light). The light-emitting layer is generally mainly composed of an organic substance that emits at least one of fluorescence and phosphorescence, or a dopant material for the organic substance and a dopant material for assisting the organic substance. Thus, the light-emitting layer is an organic layer (a layer containing an organic substance). The dopant material is added, for example, to improve the light emission efficiency and to change the light emission wavelength. The organic substance may be a low molecular compound or a high molecular compound. The thickness of the light-emitting layer is, for example, about 2nm to 200 nm.

Examples of the organic material that mainly emits at least one of fluorescence and phosphorescence include the following dye-based material, metal complex-based material, and polymer-based material.

(pigment series material)

Examples of the coloring material include cyclopentylamine derivatives, tetraphenylbutadiene derivative compounds, triphenylamine derivatives, oxadiazole derivatives, pyrazoloquinoline derivatives, distyrylbenzene derivatives, distyrylarylene (distyrylarylene) derivatives, pyrrole derivatives, thiophene ring compounds, pyridine ring compounds, perinone derivatives, perylene derivatives, oligothiophene derivatives, oxadiazole dimers, pyrazoline dimers, quinacridone derivatives, and coumarin derivatives.

(Metal complex series material)

Examples of the metal complex material include metal complexes having a rare earth metal such as Tb, EU, and Dy as a central metal, Al, Zn, Be, Ir, Pt, or the like, and having a structure of oxadiazole, thiadiazole, phenylpyridine, phenylbenzimidazole, quinoline, or the like as a ligand, and examples thereof include metal complexes having light emission from a triplet excited state such as iridium complexes and platinum complexes, hydroxyquinoline aluminum complexes, benzoquinoline beryllium complexes, benzoxazole zinc complexes, benzothiazole zinc complexes, azomethylzinc complexes, porphyrin zinc complexes, phenanthroline europium complexes, and the like.

(Polymer series Material)

Examples of the polymer material include polyparaphenylene vinylene derivatives, polythiophene derivatives, polyparaphenylene derivatives, polysilane derivatives, polyacetylene derivatives, polyfluorene derivatives, polyvinylcarbazole derivatives, and materials obtained by polymerizing the above-mentioned dye-based materials or metal complex-based light-emitting materials.

(dopant Material)

Examples of the dopant material include perylene derivatives, coumarin derivatives, rubrene derivatives, quinacridone derivatives, squarylium derivatives, porphyrin derivatives, styrene-based pigments, tetracene derivatives, pyrazolone derivatives, decacycloalkene, phenoxazinone, and the like.

The light-emitting layer can be formed by a dry film formation method, a coating method, or the like. Examples of the dry film formation method and the coating method are the same as those of the anode 42. The light-emitting layer is preferably formed by an inkjet printing method.

The organic EL section 43 may have various functional layers in addition to the light-emitting layer. Examples of the functional layer disposed between the anode 42 and the light-emitting layer are a hole injection layer, a hole transport layer, and the like. Examples of the functional layer disposed between the cathode 44 and the light-emitting layer are an electron injection layer, an electron transport layer, and the like. The electron injection layer may also be part of the cathode 44. The hole injection layer is a functional layer having a function of improving the efficiency of injecting holes from the anode 42 into the light-emitting layer. The hole transport layer is a functional layer having a function of improving the efficiency of injecting holes from the anode 42, the hole injection layer, or a portion of the hole transport layer closer to the anode 42 into the light-emitting layer. The electron transport layer is a functional layer having a function of improving electron injection efficiency from the cathode 44, the electron injection layer, or a portion of the electron transport layer closer to the cathode 44 into the light-emitting layer. The electron injection layer is a functional layer having a function of improving the efficiency of electron injection from the cathode 44 into the light-emitting layer.

Examples of the layer structure of the organic EL section 43 are as follows. In the following examples of the layer structure, the anode 42 and the cathode 44 are also shown in parentheses in order to show the arrangement relationship with the various functional layers.

(a) (Anode)/luminescent layer/(cathode)

(b) (Anode)/hole injection layer/luminescent layer/(cathode)

(c) (Anode)/hole injection layer/luminescent layer/electron injection layer/(cathode)

(d) (Anode)/hole injection layer/luminescent layer/electron transport layer/electron injection layer/(cathode)

(e) (Anode)/hole injection layer/hole transport layer/luminescent layer/(cathode)

(f) (anode)/hole injection layer/hole transport layer/luminescent layer/electron injection layer/(cathode)

(g) (anode)/hole injection layer/hole transport layer/luminescent layer/electron transport layer/electron injection layer/(cathode)

(h) (Anode)/luminescent layer/electron injection layer/(cathode)

(i) (Anode)/luminescent layer/electron transport layer/electron injection layer/(cathode)

The symbol "/" means that the layers on both sides of the symbol "/" are joined to each other.

As a material of a functional layer (for example, a hole injection layer, a hole transport layer, an electron injection layer, an electron transport layer, or the like) other than the light-emitting layer included in the organic EL section 43, a known material can be used. These functional layers may also be organic layers containing organic substances. The optimum value of the thickness of the functional layer included in the organic EL unit 43 varies depending on the material used. The thickness of the functional layer is set in consideration of conductivity, durability, and the like. The functional layers other than the light-emitting layer included in the organic EL section 43 may be formed by the same method as the light-emitting layer.

[ cathode ]

The cathode 44 is provided on the organic EL section 43. The optimum value of the thickness of the cathode 44 varies depending on the material used. The thickness of the cathode 44 is set in consideration of electrical conductivity, durability, and the like. The thickness of the cathode 44 is usually 10nm to 10 μm, preferably 20nm to 1 μm, and more preferably 50nm to 500 nm.

In order to reflect light from the organic EL unit 43 (specifically, light from the light-emitting layer) at the cathode 44 and to move the light toward the anode 42, the material of the cathode 44 is preferably a material having a high reflectance with respect to light (particularly, visible light) from the light-emitting layer of the organic EL unit 43. Examples of the material of the cathode 44 include alkali metals, alkaline earth metals, transition metals, and group 13 metals of the periodic table. As the cathode 44, a transparent conductive electrode containing a conductive metal oxide, a conductive organic substance, or the like may be used.

Examples of the method for forming the cathode 44 include coating methods such as an ink jet method, a slit coating method, a gravure coating method, a screen printing method, and a spray coating method, a vacuum deposition method, a sputtering method, and a lamination method of thermocompression bonding a metal thin film.

In the device substrate forming step S10, the device substrate 40 is formed by sequentially laminating the anode 42, the organic EL section 43, and the cathode 44 on each of the plurality of device forming regions virtually set on the substrate 41 while the strip-shaped substrate 41 is transported in the longitudinal direction in a roll-to-roll manner. The anode 42, the organic EL section 43, and the cathode 44 can be formed by the above-described method. When the organic EL section 43 has a multilayer structure, the layers may be formed in order from the anode 42 side.

[ preparation Process of sealing Member with protective film ]

In the preparation step S20 of the sealing member with the protective film (hereinafter referred to as a preparation step S20), the sealing member with the protective film 10 is heated and dehydrated in a roll-to-roll manner. As shown in fig. 2, the preparation step S20 includes a winding-out step S21, a dewatering step S22, a slow cooling step S23, and a winding-up step S24. In the present embodiment, a mode in which the slow cooling step S23 is provided between the dehydration step S22 and the winding step S24 will be described. However, the preparation step S20 may not include the slow cooling step S23.

Fig. 4 is a diagram illustrating a preparation step S20 of the sealing member with the protective film. In fig. 4, the sealing member 10 with the protective film is schematically shown by a thick solid line, and for convenience of explanation, regions related to the dehydration step S22 and the slow cooling step S23 are shown by broken lines. In the preparation step S20, the sealing member 10 of the protective film is conveyed in the longitudinal direction thereof by a plurality of conveying rollers R, and heated and dehydrated. In the conveyance of the sealing member with protective film 10, a constant tension (for example, 30N) is applied in the longitudinal direction. In the present embodiment, the sealing member 10 of the protective film is conveyed so that the protective film 30 is in contact with the conveying roller R, but the resin film 23 may be in contact with the conveying roller R.

(unwinding Process)

In the unwinding step S21, as shown in fig. 4, the roll-shaped sealing member 10 with the protective film is provided on the unwinding portion 61 disposed in the unwinding chamber 51, and then the sealing member 10 with the protective film is unwound. The rolled sealing member with the protective film 10 is conveyed to the heating chamber 52 by a conveying roller R. As shown in fig. 4, the unwinding chamber 51 and the heating chamber 52 may be directly connected or may be connected by a connection portion.

(dehydration step)

In the dehydration step S22, the sealing member 10 with the protective film conveyed from the unwinding chamber 51 is heated and dehydrated by infrared rays while being conveyed by the conveyance roller R. Specifically, the sealing member with protective film 10 is heated and dehydrated by irradiating the sealing member with protective film 10 with infrared rays from the infrared ray irradiation unit 54 disposed on the conveyance path of the sealing member with protective film 10.

The infrared irradiation unit 54 may be configured to output infrared rays for heating dehydration, and may be, for example, an infrared heater. The infrared ray irradiation unit 54 may be disposed, for example, with respect to the sealing member with protective film 10 so as to irradiate the sealing member with protective film 10 with infrared rays from the protective film 30 side.

The infrared ray irradiated to the sealing member with protective film 10 preferably contains near/mid infrared rays (wavelength 1.8 to 3.0 μm) having an absorption wavelength of water in order to efficiently heat-dehydrate the sealing member with protective film 10.

The plurality of conveyance rollers R used in the dewatering step S22 are heating rollers (rollers) R1. The temperature of the roller surface of the heat roller R1 (i.e., the heat roller R1 that comes into contact with the protective film-attached sealing member 10 heated by the infrared rays from the infrared ray irradiation section 54) is set to be equal to or higher than the glass transition temperature of the resin film 23. The temperature of the roll surface of the plurality of heating rolls R1 may be set to substantially the same temperature, and may be different as long as it is equal to or higher than the glass transition temperature of the resin film 23. The heat roller R1 is not limited as long as the temperature of the roller surface can be set to the above temperature. For example, the heating roller R1 may be configured such that a liquid (e.g., water, oil, etc.) having a temperature that can set the temperature of the roller surface to the above-described glass transition temperature or higher flows along the axis of the heating roller R1, or the heater may be incorporated in the heating roller R1. In the present embodiment, a mode in which a plurality of heating rollers R1 used in the dehydration step S22 are used has been described, but one heating roller R1 used in the dehydration step S22 may be used.

(Slow Cooling Process)

After the dehydration step S22, a slow cooling step S23 is performed in the heating chamber 52. In the slow cooling step S23, the sealing member with the protective film 10 is slowly cooled to a temperature lower than the glass transition temperature of the resin film 23 while the sealing member with the protective film 10 is conveyed by the plurality of conveying rollers R in the heating chamber 52. In the slow cooling step S23, the plurality of conveying rollers R with which the protective film-attached sealing member 10 is in contact are also the heating rollers R1, and the roller surfaces of the plurality of heating rollers R1 may be set so that the temperature decreases from a temperature equal to or higher than the glass transition temperature of the resin film 23 to a temperature lower than the glass transition temperature in stages from the upstream heating roller R1 toward the downstream heating roller R1. In this way, by changing the temperature of the roller surface of the plurality of heating rollers R1, the sealing member 10 with the protective film can be cooled slowly. In the plurality of heating rollers R1 that are gradually cooled down, the temperature of the roller surface of each heating roller R1 can be set, for example, according to the conveyance distance, conveyance speed, and the like in the slow cooling step S23. For example, in the case where the conveyance distance in the slow cooling step S23 is long, the difference in the roller surface temperature of the heating roller R1 adjacent in the conveyance direction of the sealing member with protective film 10 can be set large, and in the case where the conveyance speed is fast, the difference in the roller surface temperature of the heating roller R1 adjacent in the conveyance direction of the sealing member with protective film 10 can be set small. The conveying distance in the slow cooling step S23 may be calculated in advance by simulation, for example, or may be a distance based on actual experimental results, as long as the temperature of the resin film 23 is lower than the glass transition temperature.

In the slow cooling step S23, for example, preliminary heating may be performed at a temperature lower than that in the dehydration step S22 using the infrared irradiation unit 54 so that the temperature decreases stepwise downstream, and for example, warm air may be blown.

In the present embodiment, after the resin film 23 has a temperature lower than the glass transition temperature through the slow cooling step S23, the sealing member with protective film 10 is conveyed while being brought into contact with the conveying roller R having a roller surface temperature lower than the glass transition temperature. The temperature of the roller surface of the conveying roller R is preferably normal temperature (for example, 22 to 30 ℃).

(winding step)

In the winding step S24, the sealing member 10 with the protective film heated and dehydrated in the heating chamber 52 is wound in a roll shape by the winding portion 62 in the winding chamber 53 provided at the subsequent stage of the heating chamber 52. In the winding chamber 53, the sealing member 10 with the protective film conveyed from the heating chamber 52 is conveyed toward the winding portion 62 by the conveying roller R. As shown in fig. 4, the heating chamber 52 and the winding chamber 53 may be directly connected to each other, or they may be connected to each other by a connection portion.

[ sealing member bonding Process ]

In the sealing member bonding step S30, the protective film 30 is peeled from the protective film-attached sealing member 10 having undergone the dehydration step S22, and the sealing member 20 is bonded to the device substrate 40 via the adhesive layer 22 as shown in fig. 5, thereby obtaining an organic EL device. The sealing member bonding step S30 may be performed in a roll-to-roll manner while conveying the sealing member with protective film 10 and the device substrate 40 in the longitudinal direction, respectively.

Specifically, the roll-shaped sealing member 10 with the protective film, which is heated and dehydrated, is provided at the unwinding portion of the sealing member 10 with the protective film for the sealing member bonding step S30, which is disposed in the unwinding chamber. Then, the protective film 30 is continuously peeled off from the protective film-attached sealing member 10 while being conveyed in the longitudinal direction, with the protective film-attached sealing member 10 being wound out.

Next, the sealing member 20 obtained by peeling the protective film 30 from the protective film-attached sealing member 10 is continuously bonded to the device substrate 40 conveyed in the longitudinal direction while being conveyed in the longitudinal direction. Specifically, as shown in fig. 5, the sealing member 20 is bonded to the device substrate 40 by pressing and heating the sealing member 20 and the device substrate 40 in the thickness direction thereof in a state where the adhesive layer 22 of the sealing member 20 is opposed to the device substrate 40.

The device substrate 40 transported in the longitudinal direction may be the device substrate 40 transported continuously after the cathode 44 is formed in the device substrate forming step S10, or the device substrate 40 may be the device substrate 40 that is wound into a roll once after the cathode 44 is formed, and then is wound out after being set in a take-out section for the device substrate 40.

Although the device substrate 40 is schematically illustrated in a simplified manner in fig. 3 and 5, the anode 42 and the cathode 44 may be configured such that a part of each of the anode 42 and the cathode 44 can be drawn out from the sealing member 20 so that a voltage can be applied to the anode 42 and the cathode 44. Alternatively, electrode portions provided corresponding to the anode 42 and the cathode 44, respectively, and partially disposed outside the sealing member 20 may be formed in advance on the substrate 41, and the anode 42 and the cathode 44 may be electrically connected to the corresponding electrode portions.

Through the sealing member bonding step S30, an organic EL device is formed for each device formation region virtually set on the substrate 41. Thus, the method for manufacturing an organic EL device may further include a singulation step of singulating the substrate 41 having undergone the sealing member bonding step S30 for each device formation region. In the singulation step, the substrate 41 is divided for each device formation region, whereby an organic EL device having a product size can be obtained.

In the method for manufacturing an organic EL device, since the dehydration step S22 is provided, moisture in the sealing member 20 can be removed, and the sealing member 20 can be bonded to the device substrate 40. Therefore, a good sealing performance can be achieved, and deterioration due to moisture of an organic layer in the organic EL device can be suppressed.

In the dehydration step S22, since the moisture in the sealing member 10 with the protective film is directly heated by infrared rays, the dehydration step S22 can be performed efficiently. Further, by using infrared rays, the dehydration step S22 is easily performed while the sealing member 10 of the protective film is conveyed. This can shorten the time required for the dehydration step S22, and as a result, the productivity of the organic EL device can be improved.

In the dehydration step S22, the sealing member 10 with the protective film tends to be heated to the glass transition temperature of the resin film 23 or higher. In this case, the resin film 23 has a local change in molecular orientation. In this state, when the resin film 23 is rapidly cooled, wrinkles continuously extending in the conveying direction are generated and fixed and conspicuous. In the heating chamber 52, a plurality of conveying rollers R are generally arranged to convey the sealing member 10 of the protective film on a designed conveying path. However, the protective film-attached sealing member 10 may be slightly bent due to an error in setting the conveying roller R or the like. When such a bend occurs, the contact state with the conveying roller R in the width direction (direction orthogonal to the longitudinal direction) of the sealing member with protective film 10 becomes uneven, and wrinkles become more noticeable. If the resin film 23 is wrinkled, the sealing substrate 21 is also wrinkled accordingly. As a result, since the sealing member in which wrinkles are generated is bonded to the device substrate, air bubbles are mixed in the bonding surface, or sufficient bonding cannot be achieved due to wrinkles, and thus, there is a possibility that desired sealing performance cannot be secured.

In contrast, in the dehydration step S22 of the above-described manufacturing method, the sealing member 10 of the protective film is conveyed using the heating roller R1 in which the temperature of the roller surface is set to be equal to or higher than the glass transition temperature of the resin film 23. Thus, even if the heated sealing member with protective film 10 comes into contact with the heat roller R1, the temperature of the resin film 23 does not rapidly increase, and therefore the generation of wrinkles itself can be suppressed, and wrinkles can be suppressed from being fixed. As a result, the sealing member 20 having a desired shape in which wrinkles are suppressed can be bonded to the device substrate 40, and an organic EL device having good sealing performance can be manufactured.

The manufacturing method described in this embodiment includes a slow cooling step S23 after the dehydration step S22. In the slow cooling step S23, the protective film-attached sealing member 10 heated in the dehydration step S22 is slowly cooled, and therefore the generation of wrinkles and the fixation of wrinkles can be suppressed even between the dehydration step S22 and the winding step S24. In the embodiment in which the conveyance roller R in the slow cooling step S23 is the heating roller R1, rapid cooling due to contact between the protective film-attached sealing member 10 and the heating roller R1 does not occur even in the slow cooling step S23, and therefore generation of wrinkles and fixation of wrinkles can be suppressed.

Next, the operation and effect of the heat roller R1 will be further described with reference to examples and comparative examples.

[ example 1]

In example 1, a long sealing member a with a protective film was prepared by laminating a protective film (thickness: 12 μm), an adhesive layer (thickness: 30 μm), an aluminum foil (thickness: 30 μm), and a PET film (thickness: 38 μm) in this order. The width of the sealing member a with the protective film was 300 mm. In the protective film-attached sealing member a, the adhesive layer, the aluminum foil, and the PET film correspond to the adhesive layer 22, the sealing substrate 21, and the resin film 23 shown in fig. 1. Thus, the member obtained by peeling the protective film from the protective film-attached sealing member a is also referred to as a sealing member. The glass transition temperature of PET as a material of the PET film was 69 ℃.

The prepared sealing member a with the protective film was heated to 130 ℃ by an infrared heater while being conveyed in a heating chamber with a tension of 30N, and a dehydration step was performed. In the dehydration step, the feed roller with which the protective film-attached sealing member a is contacted is a heating roller, and the roller surface is heated to 80 ℃ with hot water. As a result, the presence or absence of wrinkles in the protective film-attached sealing member a (more specifically, the sealing member) having undergone the dehydration step was visually observed. As a result, no wrinkles were found in the sealing member a with the protective film.

In example 1, a device substrate B was further produced in which an anode layer, an organic EL unit, and a cathode layer were sequentially provided on a substrate. The organic EL unit has a multilayer structure in which a hole injection layer, a hole transport layer, a light emitting layer, an electron transport layer, and an electron injection layer are stacked from the anode layer side.

The organic EL device is manufactured by bonding a sealing member obtained by peeling the protective film from the sealing member a with the protective film having undergone the dehydration step to a device substrate B. No air bubbles were observed to be mixed into the bonding surface between the sealing member and the device substrate B, and no wrinkles were observed.

Comparative example 1

In comparative example 1, a sealing member a with a protective film having the same structure as in example 1 was prepared. In comparative example 1, a dehydration step was performed under the same conditions as in example 1, except that the temperature of the roller surface of the conveyance roller (heating roller) that was in contact with the protective film-attached sealing member a was heated to 50 ℃. As a result, in comparative example 1, wrinkles extending continuously in the conveyance direction were observed in the protective film-attached sealing member a (more specifically, the sealing member) having undergone the dehydration step.

In comparative example 1, a device substrate B having the same structure as that of example 1 was also produced. Then, a sealing member obtained by peeling the protective film from the sealing member a with the protective film subjected to the dehydration step of comparative example 1 was bonded to the device substrate B, thereby producing an organic EL device. Air bubbles are mixed into the bonding surface between the sealing member and the device substrate B, and wrinkles are generated.

[ example 2]

In example 2, a sealing member a with a protective film having the same structure as in example 1 was prepared, a dehydration step was performed under the same conditions as in example 1, and a slow cooling step was continuously performed from the dehydration step. Specifically, the temperature of the sealing member a with a protective film (more specifically, the temperature of the PET film) was slowly cooled to 60 ℃ by bringing the sealing member a with a protective film into contact with a heating roller whose roller surface was heated to 80 ℃ in a state where the sealing member a with a protective film was not heated by an infrared heater, and then conveying the sealing member a with a protective film while sequentially bringing the sealing member a with a protective film into contact with the heating roller whose roller surface was heated to 70 ℃ and the heating roller whose roller surface was heated to 60 ℃. Then, after the temperature of the sealing member a with the protective film reached 60 ℃, it was brought into contact with a conveying roller whose roller surface had a temperature of 23 ℃. As a result, no wrinkles were found in the sealing member a with a protective film (more specifically, the sealing member).

In example 2, after a device substrate B having the same structure as in example 1 was produced, a sealing member obtained by peeling the protective film from the protective film-attached sealing member a having undergone the slow cooling step was bonded to the device substrate B, thereby producing an organic EL device. No air bubbles were trapped or wrinkled on the bonding surface between the sealing member and the device substrate B.

From comparison of the results of example 1 and comparative example 1, it was verified that the occurrence of wrinkles in the protective film-attached sealing member a having undergone the dehydration step can be suppressed by the temperature of the roller surface of the conveying roller in contact with the protective film-attached sealing member a heated by the infrared heater being equal to or higher than the glass transition temperature (69 ℃) of the PET film (corresponding to the resin film 23) of the protective film-attached sealing member a. From the results of example 2, it was verified that the PET film of the sealing member a with a protective film did not wrinkle even when the slow cooling process was continuously performed after the dehydration process.

Various embodiments of the present invention have been described above. However, the present invention is not limited to the various embodiments described as examples, and is intended to include the scope described in the claims, meanings equivalent to the scope of the claims, and all modifications within the scope.

The sealing member with a protective film is described as a band, but the sealing member with a protective film may be a single sheet. Similarly, the device substrate (or the substrate included in the device substrate) may be a single sheet.

The preparation process of the sealing member with the protective film including the unwinding process and the winding process is described. However, the preparation step of the sealing member with the protective film may not include at least one of the unwinding step and the winding step. For example, the roll-out step may not be provided, and the sealing member bonding step may be continuously performed after the dehydration step while the sealing member with the protective film that has been heated and dehydrated is directly and continuously conveyed.

The method for manufacturing an organic EL device described above may further include a preliminary heating step of heating the sealing member with the protective film to a temperature equal to or higher than the glass transition temperature of the resin layer in stages before the dehydration step. In this case, the preliminary heating step is followed by the dehydration step. In the embodiment having the preheating step, the sealing member with the protective film is less likely to wrinkle during the temperature rise. In the preheating step, for example, the sealing member of the protective film is conveyed by a plurality of preheating rollers. The temperature of the roller surfaces of the plurality of preheating rollers may be set to be gradually increased from a temperature lower than the glass transition temperature of the resin layer to a temperature higher than the glass transition temperature of the resin layer from the upstream preheating roller toward the downstream preheating roller. In this case, rapid cooling of the resin layer caused by contact between the resin layer and the roller during heating can be prevented. Therefore, the sealing member with the protective film can be gradually and efficiently heated while preventing wrinkles caused by the rapid cooling. In the plurality of preheating rollers set to be raised in stages, the temperature of the roller surface of each preheating roller may be set, for example, according to the conveyance distance, conveyance speed, and the like in the preheating step. For example, when the conveyance distance in the preheating step is long, the difference between the roller surface temperatures of the preheating rollers adjacent in the conveyance direction of the sealing member with the protective film is set to be large, and when the conveyance speed is high, the difference between the roller surface temperatures of the preheating rollers adjacent in the conveyance direction of the sealing member with the protective film is set to be small. The transport distance in the preliminary heating step may be calculated in advance by simulation, or may be a distance based on actual experimental results, as long as the temperature of the resin layer is not less than the glass transition temperature. When the number of the preheating rollers used in the preheating step is three, the temperature of the roller surface of the most upstream preheating roller in the preheating step may be set to a normal temperature (for example, 22 to 30 ℃), the temperature of the roller surface of the intermediate preheating roller may be set to a temperature between the normal temperature and the glass transition temperature, and the temperature of the roller surface of the most downstream preheating roller may be set to the glass transition temperature or higher. The furthest downstream preheating roller may be shared with the furthest upstream heating roller R1 (see fig. 4) in the dehydration step. In the preliminary heating step, the sealing member with the protective film can be heated in stages while being irradiated with infrared rays.

The organic EL device manufactured by the method for manufacturing an organic EL device is not limited to the mode in which light is emitted from the substrate side, and may be applied to an organic EL device in which light is emitted from the side opposite to the substrate. Although the first electrode and the second electrode of the device substrate are described as the anode and the cathode, respectively, the first electrode may be the cathode and the second electrode may be the anode. The present invention is also applicable to organic electronic devices other than organic EL devices, for example, organic solar cells, organic photodetectors, organic transistors, and the like.

Description of reference numerals:

10 … sealing member with protective film, 20 … sealing member, 21 … sealing base material, 22 … adhesive layer, 23 … resin film (resin layer), 30 … protective film, 40 … device base material, 41 … substrate, 42 … anode (first electrode), 43 … organic EL section (device function section), 44 … cathode (second electrode), 54 … infrared irradiation section, R1 … heating roller.