CN107728358B - Method for manufacturing display device - Google Patents
Method for manufacturing display device Download PDFInfo
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- CN107728358B CN107728358B CN201710817136.5A CN201710817136A CN107728358B CN 107728358 B CN107728358 B CN 107728358B CN 201710817136 A CN201710817136 A CN 201710817136A CN 107728358 B CN107728358 B CN 107728358B
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- polyimide layer
- polyimide
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- display device
- manufacturing
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- TWNQGVIAIRXVLR-UHFFFAOYSA-N oxo(oxoalumanyloxy)alumane Chemical compound O=[Al]O[Al]=O TWNQGVIAIRXVLR-UHFFFAOYSA-N 0.000 description 1
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Images
Classifications
-
- G—PHYSICS
- G09—EDUCATION; CRYPTOGRAPHY; DISPLAY; ADVERTISING; SEALS
- G09F—DISPLAYING; ADVERTISING; SIGNS; LABELS OR NAME-PLATES; SEALS
- G09F9/00—Indicating arrangements for variable information in which the information is built-up on a support by selection or combination of individual elements
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B32—LAYERED PRODUCTS
- B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
- B32B27/00—Layered products comprising a layer of synthetic resin
-
- G—PHYSICS
- G02—OPTICS
- G02F—OPTICAL DEVICES OR ARRANGEMENTS FOR THE CONTROL OF LIGHT BY MODIFICATION OF THE OPTICAL PROPERTIES OF THE MEDIA OF THE ELEMENTS INVOLVED THEREIN; NON-LINEAR OPTICS; FREQUENCY-CHANGING OF LIGHT; OPTICAL LOGIC ELEMENTS; OPTICAL ANALOGUE/DIGITAL CONVERTERS
- G02F1/00—Devices or arrangements for the control of the intensity, colour, phase, polarisation or direction of light arriving from an independent light source, e.g. switching, gating or modulating; Non-linear optics
- G02F1/01—Devices or arrangements for the control of the intensity, colour, phase, polarisation or direction of light arriving from an independent light source, e.g. switching, gating or modulating; Non-linear optics for the control of the intensity, phase, polarisation or colour
- G02F1/13—Devices or arrangements for the control of the intensity, colour, phase, polarisation or direction of light arriving from an independent light source, e.g. switching, gating or modulating; Non-linear optics for the control of the intensity, phase, polarisation or colour based on liquid crystals, e.g. single liquid crystal display cells
- G02F1/1303—Apparatus specially adapted to the manufacture of LCDs
-
- G—PHYSICS
- G02—OPTICS
- G02F—OPTICAL DEVICES OR ARRANGEMENTS FOR THE CONTROL OF LIGHT BY MODIFICATION OF THE OPTICAL PROPERTIES OF THE MEDIA OF THE ELEMENTS INVOLVED THEREIN; NON-LINEAR OPTICS; FREQUENCY-CHANGING OF LIGHT; OPTICAL LOGIC ELEMENTS; OPTICAL ANALOGUE/DIGITAL CONVERTERS
- G02F1/00—Devices or arrangements for the control of the intensity, colour, phase, polarisation or direction of light arriving from an independent light source, e.g. switching, gating or modulating; Non-linear optics
- G02F1/01—Devices or arrangements for the control of the intensity, colour, phase, polarisation or direction of light arriving from an independent light source, e.g. switching, gating or modulating; Non-linear optics for the control of the intensity, phase, polarisation or colour
- G02F1/13—Devices or arrangements for the control of the intensity, colour, phase, polarisation or direction of light arriving from an independent light source, e.g. switching, gating or modulating; Non-linear optics for the control of the intensity, phase, polarisation or colour based on liquid crystals, e.g. single liquid crystal display cells
- G02F1/133—Constructional arrangements; Operation of liquid crystal cells; Circuit arrangements
- G02F1/1333—Constructional arrangements; Manufacturing methods
-
- G—PHYSICS
- G02—OPTICS
- G02F—OPTICAL DEVICES OR ARRANGEMENTS FOR THE CONTROL OF LIGHT BY MODIFICATION OF THE OPTICAL PROPERTIES OF THE MEDIA OF THE ELEMENTS INVOLVED THEREIN; NON-LINEAR OPTICS; FREQUENCY-CHANGING OF LIGHT; OPTICAL LOGIC ELEMENTS; OPTICAL ANALOGUE/DIGITAL CONVERTERS
- G02F1/00—Devices or arrangements for the control of the intensity, colour, phase, polarisation or direction of light arriving from an independent light source, e.g. switching, gating or modulating; Non-linear optics
- G02F1/01—Devices or arrangements for the control of the intensity, colour, phase, polarisation or direction of light arriving from an independent light source, e.g. switching, gating or modulating; Non-linear optics for the control of the intensity, phase, polarisation or colour
- G02F1/13—Devices or arrangements for the control of the intensity, colour, phase, polarisation or direction of light arriving from an independent light source, e.g. switching, gating or modulating; Non-linear optics for the control of the intensity, phase, polarisation or colour based on liquid crystals, e.g. single liquid crystal display cells
- G02F1/133—Constructional arrangements; Operation of liquid crystal cells; Circuit arrangements
- G02F1/1333—Constructional arrangements; Manufacturing methods
- G02F1/133305—Flexible substrates, e.g. plastics, organic film
-
- G—PHYSICS
- G09—EDUCATION; CRYPTOGRAPHY; DISPLAY; ADVERTISING; SEALS
- G09F—DISPLAYING; ADVERTISING; SIGNS; LABELS OR NAME-PLATES; SEALS
- G09F9/00—Indicating arrangements for variable information in which the information is built-up on a support by selection or combination of individual elements
- G09F9/30—Indicating arrangements for variable information in which the information is built-up on a support by selection or combination of individual elements in which the desired character or characters are formed by combining individual elements
-
- H—ELECTRICITY
- H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
- H05B—ELECTRIC HEATING; ELECTRIC LIGHT SOURCES NOT OTHERWISE PROVIDED FOR; CIRCUIT ARRANGEMENTS FOR ELECTRIC LIGHT SOURCES, IN GENERAL
- H05B33/00—Electroluminescent light sources
- H05B33/02—Details
-
- H—ELECTRICITY
- H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
- H05B—ELECTRIC HEATING; ELECTRIC LIGHT SOURCES NOT OTHERWISE PROVIDED FOR; CIRCUIT ARRANGEMENTS FOR ELECTRIC LIGHT SOURCES, IN GENERAL
- H05B33/00—Electroluminescent light sources
- H05B33/10—Apparatus or processes specially adapted to the manufacture of electroluminescent light sources
-
- H—ELECTRICITY
- H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
- H10K71/00—Manufacture or treatment specially adapted for the organic devices covered by this subclass
- H10K71/80—Manufacture or treatment specially adapted for the organic devices covered by this subclass using temporary substrates
-
- H—ELECTRICITY
- H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
- H10K50/00—Organic light-emitting devices
-
- H—ELECTRICITY
- H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
- H10K50/00—Organic light-emitting devices
- H10K50/80—Constructional details
-
- H—ELECTRICITY
- H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
- H10K71/00—Manufacture or treatment specially adapted for the organic devices covered by this subclass
-
- H—ELECTRICITY
- H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
- H10K71/00—Manufacture or treatment specially adapted for the organic devices covered by this subclass
- H10K71/40—Thermal treatment, e.g. annealing in the presence of a solvent vapour
- H10K71/441—Thermal treatment, e.g. annealing in the presence of a solvent vapour in the presence of solvent vapors, e.g. solvent vapour annealing
Landscapes
- Physics & Mathematics (AREA)
- Nonlinear Science (AREA)
- Engineering & Computer Science (AREA)
- General Physics & Mathematics (AREA)
- Manufacturing & Machinery (AREA)
- Optics & Photonics (AREA)
- Chemical & Material Sciences (AREA)
- Crystallography & Structural Chemistry (AREA)
- Theoretical Computer Science (AREA)
- Mathematical Physics (AREA)
- Electroluminescent Light Sources (AREA)
- Devices For Indicating Variable Information By Combining Individual Elements (AREA)
- Liquid Crystal (AREA)
- Laminated Bodies (AREA)
- Optical Filters (AREA)
- Macromolecular Compounds Obtained By Forming Nitrogen-Containing Linkages In General (AREA)
Abstract
The purpose of the present invention is to provide a method for manufacturing a display device, wherein a predetermined display portion is formed on a resin base material that is integrated with a support in advance, and then the resin base material can be easily separated from the support, thereby easily obtaining the display device. The method for manufacturing a display device is characterized in that a predetermined display part (4) is formed on a second resin layer (7) in a state that the first resin layer and the second resin layer (8) are laminated on a support (1), and then the first resin layer and the second resin layer are separated from each other at the boundary surface, thereby obtaining the display device provided with the display part on a resin substrate composed of the second resin layer.
Description
The present application is a divisional application filed on application No. 201380049620.8 entitled "method for manufacturing display device" on application date of 26/09/2013.
Technical Field
The present invention relates to a method for manufacturing a display device, and more particularly, to a method for manufacturing a display device in which a display portion is formed on a resin substrate in a liquid crystal display device, an organic EL display device, or the like.
Background
Display devices such as liquid crystal display devices and organic EL display devices are used for various displays such as large-sized displays such as televisions and small-sized displays such as cellular phones, personal computers, and smart phones. As a representative display device, there is an organic EL display device, which is manufactured, for example, by: a thin film transistor (hereinafter, TFT) is formed on a glass substrate as a supporting substrate, an electrode, a light-emitting layer, and an electrode are formed in this order, and finally, the substrate is hermetically sealed with another glass substrate, a multilayer thin film, or the like.
Here, by converting the glass substrate as the support base material from the conventional glass substrate to a resin base material, it is possible to realize a thin, light and flexible display device, and the application of the display device can be further expanded. However, resins are generally inferior to glass in dimensional stability, transparency, heat resistance, moisture resistance, gas barrier property, and the like, and thus various studies are being conducted at present.
For example, patent document 1 relates to an invention relating to a polyimide and a precursor thereof useful as a plastic substrate for a flexible display, and reports that a polyimide obtained by reacting various diamines with tetracarboxylic acids having an alicyclic structure such as cyclohexylphenyltetracarboxylic acid has excellent transparency. Further, attempts have been made to reduce the weight by using a flexible resin as a supporting substrate, and for example, non-patent documents 1 and 2 below propose an organic EL display device using a polyimide having high transparency as a supporting substrate.
As described above, although resin films such as polyimide are known to be useful for plastic substrates for flexible displays, the manufacturing process of display devices has been carried out using glass substrates, and most of the production facilities thereof have been designed on the premise of using glass substrates. Accordingly, it is desirable to produce a display device while effectively utilizing existing production equipment.
As a specific example of the study, the following production method is known: a display device having a display portion on a resin base is manufactured by completing a predetermined manufacturing process of the display device in a state where a resin film is laminated on a glass substrate and then removing the glass substrate (see patent document 2, non-patent document 3, and non-patent document 4). In these cases, the resin substrate and the glass must be separated from each other without damaging a display portion (display portion) formed on the resin substrate.
That is, in non-patent document 3, after a predetermined display portion is formed on a resin substrate that is applied to and fixed on a glass substrate, a Laser is irradiated from the glass side by a method called an EPLaR (Laser on Plastic by Laser Release) process, and the resin substrate having the display portion is forcibly separated from the glass. However, this method has a disadvantage of low productivity because it requires an expensive laser device and takes time for separation. Further, the surface properties of the resin base material and the display unit mounted thereon may be adversely affected during the separation.
On the other hand, the method described in non-patent document 4 is a method for improving the disadvantages of the EPLaR method, and the method is as follows: after a release layer is formed by coating on a glass substrate, a polyimide resin is coated on the release layer, and after the manufacturing process of the organic EL display device is completed, the polyimide film layer is released from the release layer. Fig. 1 and 2 show a method for manufacturing an organic EL display device described in non-patent document 4. The method comprises the following steps: after a release layer 2 is formed on a glass substrate 1, a polyimide layer 3 is formed one turn larger than the release layer 2, and then, a process treatment of a predetermined TFT and organic EL step is performed to form a TFT/organic EL panel portion (display portion) 4, and then, the polyimide layer 3 and the TFT/organic EL panel portion (display portion) 4 are separated from the release layer 2 by cutting the release layer 2 along a cutting line 5 on the inner side of the release layer 2. However, non-patent document 4 does not specifically describe what material is used for the release layer. Therefore, it is not clear in practice what degree of force is required for separation from the release layer and what state the surface properties of the separated polyimide layer 3 are. In addition, since the area of the peeling layer needs to be made smaller than that of the polyimide layer, the formable area of the organic EL display device is limited, and productivity is a problem. If the area of the release layer is increased to prevent a decrease in productivity, the area of the polyimide layer bonded to the glass at the outer periphery of the release layer is decreased, and peeling is likely to occur due to stress in the process.
The method described in patent document 2 is as follows: after a release layer made of Parylene (Parylene) or cyclic olefin copolymer is formed on a glass substrate, a polyimide layer is formed one turn larger than the release layer in the same manner as in the method described in non-patent document 4, and after fabrication of an electronic device thereon, the polyimide layer is peeled. In general, the formation of a TFT required for display applications requires an annealing step of about 400 ℃, but in this method, the heat resistance of the release layer is inferior to that of polyimide, and therefore, there is a problem that the heat treatment temperature of the polyimide layer and the maximum temperature at the time of manufacturing an electronic device are limited by the heat resistance of the release layer. Further, since the adhesion between the glass and the peeling layer and between the peeling layer and the polyimide layer is weak, the glass cannot withstand the stress in the process, and may cause peeling. Further, the thermal expansion coefficient of the release layer is larger than that of polyimide, and a difference in thermal expansion coefficient depending on the kind of resin may cause warpage.
The methods described in these patent documents 2 to 3 and non-patent documents 3 to 4 both use glass as a support and form a display portion on a resin base material fixed to the glass, thereby ensuring the operability and dimensional stability of the resin base material and having an advantage that a glass substrate can be used directly on an existing production line for manufacturing display devices such as liquid crystal display devices and organic EL display devices. Therefore, if separation can be extremely easily performed after forming a predetermined display portion without affecting the resin base material and the display portion, not only is a method excellent in mass productivity, but also transition from the glass substrate to the resin base material can be further promoted.
Documents of the prior art
Patent document
Patent document 1: japanese laid-open patent publication No. 2008-231327
Patent document 2: japanese laid-open patent publication No. 2010-67957
Patent document 3: japanese patent laid-open publication No. 2009-21322
Non-patent document
Non-patent document 1: s.an et.al. "2.8-inch WQVGA Flexible AMOLED Using High Performance Low Temperature Polysilicon TFT on Plastic Substrates", SID2010DIGEST, p706(2010)
Non-patent document 2: oishi et al, "transmissive PI for flexible display", IDW' 11FLX2/FMC4-1
Non-patent document 3: "Flexible OLED display Made with the EPLaR Process", Proc. Eurodisplay' 07, pp.36-39(2007)
Non-patent document 4: Cheng-Chung Lee et al, "A Novel Approach to Make Flexible Active Matrix Displays", SID10Digest, pp.810-813(2010)
Disclosure of Invention
Therefore, an object of the present invention is to provide a method for easily obtaining a display device by forming a predetermined display portion on a resin base material integrated with a support in advance and then easily separating the resin base material from the support.
As a result of studies to solve the above problems, the present inventors have found that a display device including a display portion on a resin substrate made of a second resin layer can be obtained extremely easily by forming a predetermined display portion on the second resin layer in a state where the first resin layer and the second resin layer are laminated on a support and then separating the display portion at a boundary surface between the first resin layer and the second resin layer, and have completed the present invention.
That is, the gist of the present invention is as follows.
(1) A method for manufacturing a display device, characterized in that a predetermined display portion is formed on a second resin layer in a state where the first resin layer and the second resin layer are laminated on a support, and thereafter, a boundary surface between the first resin layer and the second resin layer is separated, thereby obtaining a display device having a display portion on a resin base material made of the second resin layer.
(2) The method of manufacturing a display device according to (1), wherein a laminated film in which a first resin layer and a second resin layer are directly laminated is laminated to a support, that is, a first resin layer surface of the laminated film is laminated to one surface of the support via an adhesive layer, a predetermined display portion is formed on the laminated film, and thereafter, a boundary surface between the first resin layer and the second resin layer is separated, thereby obtaining a display device including a display portion on a resin base material made of the second resin layer.
(3) The method of manufacturing a display device according to (2), wherein the first resin layer and the second resin layer constituting the laminated film are each made of polyimide.
(4) The method of manufacturing a display device according to (1), wherein the first polyimide layer and the second polyimide layer are formed on the support, and then a predetermined display portion is further formed, and thereafter, the first polyimide layer and the second polyimide layer are separated at the boundary surface, thereby obtaining a display device having a display portion on the polyimide substrate made of the second polyimide layer.
(5) The method for manufacturing a display device according to item (4), wherein the display device having the display portion on the polyimide substrate is obtained by removing the support after forming the predetermined display portion and then separating the first polyimide layer and the second polyimide layer at the boundary surface.
(6) The method of manufacturing a display device according to (4) or (5), wherein the formation of the first polyimide layer is performed by laminating polyimide films, and the formation of the second polyimide layer is performed by applying a resin solution of polyimide or a polyimide precursor.
(7) The method for manufacturing a display device according to (4) or (5), wherein the formation of the first polyimide layer and the second polyimide layer is performed by applying and heating a resin solution of polyimide or a polyimide precursor.
(8) The method of manufacturing a display device according to any one of (4) to (7), wherein a part of the second polyimide layer protrudes from a peripheral portion of the first polyimide layer, and the protruding portion of the second polyimide layer is fixed to the support.
(9) The method of manufacturing a display device according to any one of (4) to (7), wherein a part of one of the first polyimide layer and the second polyimide layer protrudes from a peripheral portion of the other layer.
(10) The method of manufacturing a display device according to any one of (4) to (9), wherein the first resin layer and the second resin layer are separated after the slit is cut into the first resin layer along the outer periphery of the display portion.
(11) According to the method for manufacturing a display device described in (6) or (7), when the formation of the second polyimide layer is performed by heating after coating the resin solution of polyimide or a polyimide precursor, the high-temperature retention time of the second polyimide layer is less than 60 minutes.
(12) The method of manufacturing a display device according to any one of (1) to (11), wherein the support is a glass substrate.
(13) The method of manufacturing a display device according to any one of (1) to (12), wherein a thermal expansion coefficient of the first resin layer is 25ppm/K or less.
(14) The method of manufacturing a display device according to any one of (1) to (13), wherein a thermal expansion coefficient of the second resin layer is 25ppm/K or less.
(15) The method for manufacturing a display device according to any one of (1) to (14), wherein a transmittance of the second resin layer in a wavelength region of 440nm to 780nm is 80% or more.
(16) The method of manufacturing a display device according to any one of (1) to (15), wherein the display portion is formed with the gas barrier layer interposed therebetween, and a difference in thermal expansion coefficient between the second resin layer and the gas barrier layer is 10ppm/K or less.
(17) The method of manufacturing a display device according to any one of (1) to (16), wherein the display portion is a color filter layer.
(18) The method for manufacturing a display device according to any one of (1) to (17), wherein a peel strength of the first resin layer and the second resin layer is 200N/m or less.
(19) The method for manufacturing a display device according to any one of (1) to (18), wherein at least one of the first resin layer and the second resin layer is made of polyimide having a structural unit represented by general formula (1).
[ wherein Ar is1Represents a group having a valence of 4 to an aromatic ringOrganic radical, Ar2Is a 2-valent organic group represented by the following general formula (2) or (3).
[ herein, R in the general formula (2) or the general formula (3)1～R8Each independently represents a hydrogen atom, a fluorine atom, an alkyl group or alkoxy group having 1 to 5 carbon atoms, or a fluorine-substituted hydrocarbon group, R in the general formula (2)1～R4At least 1 of (a) and R of the formula (3)1～R8At least 1 of them is a fluorine atom or a fluorine-substituted hydrocarbon group. Angle (c)]
According to the present invention, by forming the first resin layer and the second resin layer in advance in a state of being laminated on the support, it is possible to form a predetermined display portion while securing operability and dimensional stability. After the display portion is formed, the first resin layer and the second resin layer can be easily separated from each other by the interface without particularly performing laser irradiation or the like, and thus a display device can be obtained extremely easily. Further, since the second resin layer serving as the resin base material and the display portion are not affected after the separation and the support is not damaged, the support can be reused in the manufacture of the display device, which contributes to a significant reduction in manufacturing cost.
Drawings
Fig. 1 is a schematic diagram illustrating a method of manufacturing an organic EL display device in the related art.
Fig. 2 is a schematic diagram illustrating a method of manufacturing an organic EL display device according to the related art.
Fig. 3 is a schematic diagram illustrating a method of manufacturing a display device according to the present invention.
Fig. 4 is a schematic diagram illustrating a method of manufacturing a display device according to the present invention.
Fig. 5 is a schematic view (partially enlarged) illustrating a method for manufacturing a display device according to the present invention.
Fig. 6 is a schematic diagram illustrating a method of manufacturing a display device according to the present invention.
Fig. 7 is a schematic diagram illustrating a method of manufacturing a display device according to the present invention.
Fig. 8 is a schematic diagram illustrating a method of manufacturing a display device according to the present invention.
Fig. 9 is a schematic diagram illustrating a method of manufacturing a display device according to the present invention.
Detailed Description
The present invention will be described in more detail below with reference to the accompanying drawings, but the present invention is not limited to the following description.
In the method for manufacturing a display device according to the present invention, a predetermined display portion is formed on the second resin layer in a state where the first resin layer and the second resin layer are laminated on the support, and thereafter, the first resin layer and the second resin layer are separated at a boundary surface therebetween, thereby obtaining a display device including a display portion on the resin base material made of the second resin layer. The details are described below. In the following, a case where both the first resin layer and the second resin layer are formed of polyimide will be described as a preferable example, but at least one of the resin layers may be formed of a resin other than polyimide.
In the method for manufacturing a display device of the present invention, a member having a first polyimide layer and a second polyimide layer provided on a support in advance is used. Then, a predetermined display portion is formed on the second polyimide layer side, and thereafter, a boundary surface between the first polyimide layer and the second polyimide layer is separated, whereby a display device having a display portion on a resin base material (polyimide base material) made of the second polyimide layer can be manufactured.
More specifically, as shown in fig. 3, a support 1 serving as a base in a process of manufacturing a display unit of a liquid crystal display device, an organic EL display device, or the like is prepared. The support 1 is not particularly limited as long as it has chemical strength and mechanical strength capable of withstanding thermal history, atmosphere, and the like in a manufacturing process of forming a display unit of various display devices, and a glass substrate or a metal substrate can be exemplified, and a glass substrate is preferably used. As the glass substrate, for example, a glass substrate generally used in the production of an organic EL display device can be used. However, in the display device manufactured by the present invention, the support substrate of the display portion is a polyimide substrate composed of the second polyimide layer 8. In other words, the glass substrate mentioned here is a member that functions as a base when forming a display portion on a polyimide base material, and the handling property, dimensional stability, and the like of the polyimide base material are ensured in the manufacturing process of the display portion, but are finally removed without constituting a display device. The support may be subjected to a surface treatment for controlling the releasability of the first polyimide layer 7 and the second polyimide layer 8.
In the present invention, the first polyimide layer and the second polyimide layer are provided on the support 1, and any one of the following methods may be used as a method therefor: 1) a method (lamination method) of laminating a first polyimide layer and a second polyimide layer in advance and then laminating the laminated polyimide laminate film on a support; 2) a method (coating method) of forming a first polyimide layer and a second polyimide layer by coating a resin solution of polyimide or a polyimide precursor (hereinafter, also referred to as "polyamic acid"); 3) a method (combination method) in which a first polyimide layer is formed by laminating a polyimide film on a support, and a second polyimide layer is formed by applying a resin solution of polyimide or a polyimide precursor. Here, the support 1 and the first polyimide layer may be directly laminated by adhesion, or may be laminated via an adhesive layer as shown in fig. 3.
In the present invention, at least a part of any one of the first polyimide layer and the second polyimide layer may be formed so as to protrude from a peripheral portion of the other layer. By providing a thin portion of the polyimide layer in the peripheral portion outside the portion where the display portion is formed, stress generated in the process can be dispersed, and separation of the support and the polyimide layer in the process can be prevented. The protrusion distance is not particularly limited, and is preferably not less than the total thickness of the first polyimide layer and the second polyimide layer, and more preferably not less than 10 times the total thickness thereof.
Hereinafter, the above-mentioned 3 methods will be described.
< lamination method >
Fig. 3 is a view showing a state in which a polyimide laminate film is attached to the support 1 by the adhesive layer 6 and the display section is further laminated. Here, the polyimide laminated film is composed of a first polyimide layer 7 and a second polyimide layer 8, and the first polyimide layer 7 and the second polyimide layer 8 are directly laminated in advance. To obtain such a polyimide laminate film, for example, a method (casting method) may be mentioned in which a resin solution of polyamic acid to be the second polyimide layer 8 is applied to a polyimide film to be the first polyimide layer 7, and then dried and imidized by heat treatment. As the adhesive layer 6, in addition to a resin adhesive such as an epoxy resin or an acrylic resin, an adhesive film having adhesive layers provided on both surfaces of a support film, or the like can be used. In addition, although the adhesive layer 6 is used in fig. 3, the first polyimide layer 7 side may be directly bonded to the support 1 by a method such as heat pressure bonding, as shown in fig. 7.
Here, the thickness of the second polyimide layer 8 constituting the laminated film is preferably 3 μm to 50 μm. If the thickness of the second polyimide layer 8 is less than 3 μm, it is difficult to secure electrical insulation when forming a resin substrate of a display device, prevent damage of the resin layer due to external factors, and the like, whereas if it exceeds 50 μm, flexibility, transparency, and the like of the display device may be reduced. On the other hand, the first polyimide layer 7 is preferably 10 μm or more in view of handling as a laminated film, since it does not directly constitute a display device. The upper limit of the thickness is not particularly limited, but is preferably 100 μm or less in consideration of cost and the like.
As described above, the polyimide laminated film is laminated and integrated on the support 1 via the adhesive layer 6 or without the adhesive layer 6, and the process proceeds to the step of forming the display unit. Here, the step of forming the display portion refers to a predetermined TFT/organic EL step process in the case of an organic EL display device, for example, and the TFT, the organic EL element including an electrode and a light-emitting layer, and the like formed by the process correspond to the display portion. Here, an organic EL that performs color display by combining a color filter with an organic EL that emits white light has also been proposed. The color filter is manufactured by forming the color filter in a different way from the TFT/organic EL process and then attaching the color filter to the TFT/organic EL side, and the color filter also corresponds to a display portion. In the case of a liquid crystal display device, the process refers to a TFT process, and a TFT, a driver circuit, a color filter, and the like formed by the process correspond to a display portion. That is, the process of forming a display unit, including various display devices such as electronic paper and MEMS displays, in addition to organic EL display devices and liquid crystal display devices, conventionally refers to a process of forming various functional layers formed on a glass substrate, that is, a process of reflecting members necessary for a predetermined image (moving image or image), and members obtained thereby, including the display unit, are collectively referred to as a display unit. Through this step, the display portion 4 is laminated and formed on the second polyimide layer 8 side integrated with the first polyimide layer 7. After all the display portion laminating steps are completed, a cutting step of cutting the display portion into a predetermined size is performed.
Fig. 4 is a diagram showing a dicing step. In the present invention, the cutting step is not essential, and may be performed arbitrarily according to the apparatus and the process of manufacture. When the manufacturing of the organic EL display device is described as an example, the dicing is performed along the dicing line 5 shown in fig. 4 to the display portion (TFT/organic EL panel portion) 4 and the second polyimide layer 8. At this time, as shown in fig. 5 showing an enlarged view of the cut region 9 shown in fig. 4, if the cutting line 10 is cut into the first resin layer along the outer periphery of the display portion while reaching the vicinity of the center of the first polyimide layer 7, the second polyimide layer 8 can be reliably and easily separated from the boundary surface with the first polyimide layer 7 without causing mechanical damage to the TFT/organic EL panel portion 4.
Here, in order to easily separate the second polyimide layer 8 from the interface with the first polyimide layer 7, it is necessary to make the polyimide interface in a state of being easily peeled off. The mode is not particularly limited, and polyimide having a specific chemical structure is used for at least one of the first and second polyimide layers.
Generally, polyimide is obtained by polymerizing an acid anhydride and a diamine as raw materials, and is represented by the following general formula (1).
In the formula, Ar1Represents an organic group having a valence of 4, Ar, as an acid anhydride residue2Is a 2-valent organic group as a diamine residue, but Ar is preferred from the viewpoint of heat resistance1、Ar2At least one of them is an aromatic residue.
Examples of the polyimide resin preferably used for the first polyimide layer or the second polyimide layer in the present invention include a polyimide having the following repeating structural unit,
particularly preferred is polyimide having the following repeating structural unit.
In addition to these, fluorine-containing polyimide may be mentioned. Here, the fluorine-containing polyimide is a polyimide having a fluorine atom in a polyimide structure, and at least one of an acid anhydride and a diamine as raw materials of the polyimide has a fluorine-containing group. Examples of the fluorine-containing polyimide include the following compounds: in the polyimide represented by the above general formula (1), Ar in the formula1Is a 4-valent organic radical, Ar2Is a 2-valent organic group represented by the following general formula (2) or (3).
R in the above general formula (2) or general formula (3)1～R8Each independently represents a hydrogen atom, a fluorine atom, an alkyl group or alkoxy group having 1 to 5 carbon atoms, or a fluorine-substituted hydrocarbon group, R in the general formula (2)1～R4ToAt least 1 of which is a fluorine atom or a fluorine-substituted hydrocarbon group, and R of the general formula (3)1～R8At least 1 of them is a fluorine atom or a fluorine-substituted hydrocarbon group.
Wherein, as R1～R8Preferable specific examples of (A) include-H and-CH3、-OCH3、-F、-CF3Etc., but it is preferred that at least 1 substituent in formula (2) or formula (3) is-F or-CF3Any one of them.
Ar in the general formula (1) for forming a fluorine-containing polyimide1Specific examples of (3) include the following 4-valent acid anhydride residues.
In addition, when the fluorine-containing polyimide is formed, Ar in the general formula (1) is given in consideration of transparency of polyimide, releasability from other layers, and the like2The specific diamine residue of (3) is preferably as follows.
With such a fluorine-containing polyimide, good separability can be exhibited even at the interface with a polyimide having a structure other than the fluorine-containing polyimide (naturally, if both the first and second polyimide layers are fluorine-containing polyimides, the separability at the interface is further improved). In addition, when any of the structural units represented by the following general formulae (4) or (5) is contained in such a fluorine-containing polyimide in a proportion of 80 mol% or more, the polyimide is excellent in transparency and peelability, and is low in thermal expansibility and excellent in dimensional stability, and therefore, is preferably used as a polyimide for forming the second polyimide layer.
When the polyimide is a polyimide having a structure of the general formula (4) or (5), the polyimide other than the polyimide which can be added in a proportion of less than 20 mol% at the maximum is not particularly limited, and a general acid anhydride and diamine can be used. Among them, preferable examples of the acid anhydride include pyromellitic dianhydride, 3 ', 4,4 ' -biphenyltetracarboxylic dianhydride, 1, 4-cyclohexanedicarboxylic acid, 1,2,3, 4-cyclobutanetetracarboxylic dianhydride, and 2,2 ' -bis (3, 4-dicarboxyphenyl) hexafluoropropane dianhydride. On the other hand, examples of the diamine include 4,4 ' -diaminodiphenyl sulfone, trans-1, 4-diaminocyclohexane, 4 ' -diaminocyclohexylmethane, 2 ' -bis (4-aminocyclohexyl) -hexafluoropropane, 2 ' -bis (trifluoromethyl) -4,4 ' -diaminobicyclohexyl and the like.
The various polyimides described above are obtained by imidizing a polyamic acid, and a resin solution of the polyamic acid can be obtained by reacting a diamine and an acid dianhydride, which are raw materials, in an organic solvent in substantially equimolar amounts. More specifically, the diamine can be obtained by dissolving a diamine in an organic polar solvent such as N, N-dimethylacetamide under a nitrogen stream, adding tetracarboxylic dianhydride, and reacting at room temperature for about 5 hours. The weight average molecular weight of the obtained polyamic acid is preferably 1 to 30 ten thousand from the viewpoints of uniformity of film thickness at the time of coating and mechanical strength of the obtained polyimide film. The preferable molecular weight range of the polyimide layer is also the same as that of the polyamic acid.
In the present invention, it is preferable that the second polyimide layer 8 is a polyimide having a structural unit represented by the general formula (4) or (5), so that a polyimide layer having a thermal expansion coefficient of 25ppm/K or less, preferably 10ppm/K or less can be formed, and the polyimide layer is suitable as a polyimide substrate for forming a display device. The polyimide having these structural units has a glass transition temperature (Tg) of 300 ℃ or higher, and has a transmittance of 80% or higher in a wavelength region of 440nm to 780 nm.
As described above, in order to allow a predetermined polyimide to be used and to allow the first polyimide layer and the second polyimide layer to be easily separated from each other at the interface, it is preferable that at least one of the polyimide layers is formed of a fluorine-containing polyimide. When at least one polyimide layer is formed of a fluorine-containing polyimide, the adhesive strength at the interface between the first polyimide layer and the second polyimide layer is preferably 1N/m to 500N/m, more preferably 5N/m to 300N/m, and even more preferably 10N/m to 200N/m, and therefore, the polyimide film has separability to such an extent that the polyimide film can be easily peeled off by a human hand. In the display device obtained by the separation, the second polyimide layer as the polyimide substrate has no appearance defects such as wrinkles and cracks, and the separation surface of the second polyimide layer can maintain the surface roughness (generally, the surface roughness Ra is about 1 to 80 nm) obtained by the casting method, and therefore, the visibility of the display device and the like are not adversely affected.
The present invention includes a method of 1) forming a predetermined display portion and then separating the first polyimide layer and the second polyimide layer at the boundary surface, and the method further includes: 2) after a predetermined display portion is formed, the support on the first polyimide layer side is removed, and then the interface between the remaining first polyimide layer and the second polyimide layer is separated, thereby obtaining a display device having a display portion on a polyimide substrate (second polyimide layer). In the method of 2) above, the first polyimide layer 7 and the second polyimide layer 8 are preferably separated while the shape of the second polyimide layer 8 and the shape of the display portion 4 are fixed so as to be constant during the separation, after the support 1 is removed, and the first polyimide layer 7 is preferably separated. This can reduce the stress to which the display unit 4 is subjected, and can reduce the possibility of damage to the device of the display unit 4 even when the second polyimide layer 8 is made thinner. Here, in the method 2), the method for removing the support is not particularly limited as long as the display portion 4 and the second polyimide layer 8 are not damaged, and the following method can be used. That is, since the above description based on fig. 3 shows an example in which the adhesive layer 6 is used, this point will be supplemented in the description based on the coating method of fig. 6. However, in the lamination method, if the first polyimide layer 7 can be directly bonded to the support 1 by a method such as thermocompression bonding, the need for the adhesive layer 6 as in fig. 3 is eliminated, and in this case, the support 1 can be removed by a method similar to that described later.
Next, an application example of the coating method according to the present invention will be described.
< coating method >
Fig. 6 is a view showing a state in which the first polyimide layer 7 and the second polyimide layer 8 are sequentially formed on the support 1 by a coating method, and then the display unit 4 is further laminated. In this method, first, the support 1 is prepared, a resin solution of polyamic acid to be the first polyimide layer 7 is applied thereon, and the first polyimide layer 7 is formed by heat treatment, drying, and imidization. Next, a resin solution of polyamic acid to be the second polyimide layer 8 is applied to the first polyimide layer 7, and then dried and imidized by heat treatment, thereby forming the second polyimide layer 8. This enables the substrate to be produced in which the first polyimide layer 7 and the second polyimide layer 8 are formed in this order on the support 1. Thereafter, the process continues after the display portion forming process. The steps after the display portion forming step are the same as those in the above-described lamination method, and therefore, the details are omitted, and the removal of the support 1 in the method of 2) above will be briefly described below.
As described above, fig. 6 is a diagram showing a state in which the first polyimide layer 7, the second polyimide layer 8, and the display unit 4 are laminated on the support 1. In the present invention, the support 1 can be removed from this state to before the step of separating the boundary surface between the first polyimide layer 7 and the second polyimide layer 8, and here, as a method of removing the support 1, the following method can be exemplified: a polyimide material which is easily peeled from the support 1 is used as the first polyimide layer 7, or a metal foil such as a copper foil or a metal substrate is used as the support 1, and these are removed with an etching solution.
As a method for removing the support 1, other known methods may be used. That is, the support 1 can be removed by laser irradiation in non-patent document 3 or the release layer in non-patent document 4. When the support 1 is removed by laser irradiation, the first polyimide layer absorbs the laser beam, and adverse effects of the laser beam on the 2 nd polyimide layer and the display portion can be prevented. When the support 1 is removed by the peeling layer, the first polyimide layer functions as a stress relaxation layer against stress generated at the time of peeling, and a decrease in yield due to damage to the display portion at the time of peeling can be prevented.
However, japanese patent application laid-open No. 2007 and 512568 disclose that a yellow film of polyimide or the like is formed on a glass, a thin-film electronic element is formed on the yellow film, and then a bottom surface of the yellow film is irradiated with a UV laser beam through the glass, whereby the glass and the yellow film can be peeled off. However, it is also disclosed that, unlike the yellow film, since a transparent plastic does not absorb UV laser light, an absorption/release layer such as amorphous silicon needs to be provided under the film in advance. On the other hand, Japanese patent laid-open No. 2012-511173 discloses that in order to peel a glass from a polyimide film by UV laser irradiation, it is necessary to use a laser beam having a spectrum in the range of 300 to 410 nm.
In the present invention, when the support is removed from the first polyimide layer by laser light, colored polyimide is preferably used for the first polyimide layer. It is one of preferable modes of the present invention to use colored polyimide as the first polyimide layer and transparent polyimide as the second polyimide layer.
In the coating method, a resin solution of polyamic acid to be the first polyimide layer 7 is coated on the support 1, and heat treatment is performed, and at this time, the first polyimide layer is imidized by sufficient heat treatment to facilitate separation of the second polyimide layer, which is preferable. In the coating method, as described in the lamination method, polyimide having a specific chemical structure is preferably used for at least one of the first and second polyimide layers. The first polyimide layer and the second polyimide layer may be made of polyimide of the same chemical structure.
In the coating method, the first polyimide layer and the second polyimide layer are each obtained by applying a resin solution and then drying or drying and curing the resin solution by heat treatment, and in the present invention, the heating time (hereinafter referred to as high-temperature holding time) in the high-temperature heating temperature region from a temperature lower by 20 ℃ than the maximum heating temperature (maximum reaching temperature) at the time of temperature rise in the heat treatment is preferably shorter within a range in which desired characteristics are obtained. This is because the purpose of holding the first and/or second polyimide layer in a high-temperature heating temperature region in the coating method is to obtain the characteristics required for the original polyimide layer by promoting complete removal of the residual solvent, orientation of the polyimide resin, and the like. However, if the high-temperature holding time of the second polyimide layer is particularly long, the releasability from the first polyimide layer tends to decrease, or the transmittance tends to decrease due to coloring or the like. The optimum high-temperature holding time varies depending on the heating method, the thickness of the polyimide, and the type of polyimide, and is preferably 0.5 minutes or more and less than 60 minutes, and more preferably 0.5 minutes or more and less than 30 minutes.
Next, an application example of a combined use of the film laminate of the present invention and a resin solution coating method will be described.
< Combined use >
Fig. 8 is a diagram showing a state where the first polyimide layer 7 is attached to the support 1 by the adhesive layer 6, and the second polyimide layer 8 and the display section 4 are stacked thereon, wherein the first polyimide layer 7 is cut one turn smaller than the support 1.
In this method, first, the support 1 is prepared, and a polyimide film to be the first polyimide layer 7 is attached thereto by the adhesive layer 6. This step may be carried out using the same polyimide film as the above-mentioned lamination method, and the same method is used.
Next, a resin solution of polyamic acid to be the second polyimide layer 8 is applied to the first polyimide layer 7, and is dried by heat treatment to complete imidization, thereby forming the second polyimide layer 8. The same resin solution as the above coating method can be used for this step, and the same method can be used. This enables the substrate to be produced in which the first polyimide layer 7 and the second polyimide layer 8 are formed in this order on the support 1. Thereafter, the process continues after the display portion forming process. The steps after the display portion forming step are the same as those described above, and therefore, are omitted.
In the combined use, after the first polyimide layer 7 and the support 1 are bonded, a resin solution of polyamic acid to be applied to the second polyimide layer 8 is applied in a varnish state to the first polyimide layer 7 so as to cover the entire surface thereof. The resin solution of the applied polyamic acid is dried and imidized by heat treatment to form the second polyimide layer 8, and as shown in fig. 8, the lamination surface of the second polyimide layer 8 is larger than that of the first polyimide layer in this state, and at least a part of the portion of the second polyimide layer 8 not in contact with the first polyimide layer 7 is in contact with the support 1. That is, a part of the second polyimide layer 8 protrudes from the peripheral portion of the first polyimide layer 7, and the protruding portion of the second polyimide layer 8 is fixed to the support 1. In this method, the second polyimide layer 8 and the first polyimide layer 7 are also configured to be easily peeled off, but since the second polyimide layer 8 and the support 1 can be firmly bonded by the protruding portion of the second polyimide layer 8, the adhesiveness can be improved around the support, and the stability in the process can be further ensured. After the display portion is formed, the same process as the dicing process described above may be performed, and for example, as shown in fig. 9, if the display portion 4 and the second polyimide layer 8 are diced along the dicing lines 5 from which the display portion 4 is cut, and the display portion 4 is separated from the interface between the first polyimide layer 7 and the second polyimide layer 8, a display device including the display portion 4 on the polyimide substrate made of the second polyimide layer 8 can be obtained.
In the present invention, the first polyimide layer is separated after the first polyimide layer is separated, including the case of using the 3 methods described above and the case of using a method other than these methods, and therefore does not contribute to the function of the display device, but the thermal expansion coefficient of the first polyimide layer is preferably 25ppm/K or less, from the viewpoint that the characteristics before the separation become important in consideration of the temperature change of the display portion at the time of the manufacturing process. Further, the glass transition temperature Tg is preferably 300 ℃ or higher. Specific examples of such a first polyimide layer include, for example, polyimides containing, as main components, a structural unit composed of biphenyltetracarboxylic dianhydride and phenylenediamine. Examples of commercially available products include UPILEX-S manufactured by Utsu Kagaku K.K., KAPTON manufactured by DU PONT-TORAY K.K., and XENOMAX manufactured by Toyo Boseki K.K.
In the present invention, a gas barrier layer having a barrier property against oxygen, water vapor, or the like, which is formed of an inorganic oxide film such as silicon oxide, aluminum oxide, silicon carbide, silicon oxycarbide, silicon carbonitride, silicon nitride, or silicon oxynitride, or the like, can be used for forming the display portion. In this case, in order to reduce warpage and the like of the obtained display device, the difference in thermal expansion coefficient between the second polyimide layer and the gas barrier layer is preferably 10ppm/K or less.
In order to enable easy separation of the first polyimide layer 7 and the second polyimide layer 8 from the boundary surfaces thereof in a method other than using a polyimide having a specific chemical structure for the first or second polyimide layer, for example, a method using a laminated film produced by: after the surface state of the first polyimide layer 7 is changed by heat treatment or the like of the first polyimide layer 7 to reduce the wettability of the surface, the second polyimide layer 8 is coated quickly. The appropriate temperature for this heat treatment varies depending on the type of the first polyimide layer 7, and is preferably 300 to 500 ℃ when the first polyimide layer 7 is a polyimide film such as KAPTON manufactured by DU PONT-TORAY Co., Ltd., and UPILEX manufactured by UK.K.K.K..
In the method of separating the interface between the first polyimide layer and the second polyimide layer after forming the predetermined display portion, the second polyimide layer is formed again on the first polyimide layer side of the laminate of the support obtained by separating the second polyimide layer and the first polyimide layer, whereby the laminate of the support and the first polyimide layer can be reused. When used repeatedly, the cleaning of the laminate of the support and the first polyimide layer may be performed after the separation of the second polyimide layer. Further, the heat treatment of the laminate of the support and the first polyimide layer may be performed to reduce the wettability of the surface of the first polyimide layer, and then the coating of the second polyimide layer may be performed.
As another method of reusing the laminate of the support and the first polyimide layer, the following method may be used: the first polyimide layer is formed again on the first polyimide layer side of the laminate of the support obtained by separating the second polyimide layer and the first polyimide layer, and thereafter the second polyimide layer is formed.
In the present invention, the support removed from the first polyimide layer may be reused. Before reuse, the support may be cleaned, heat treated, and surface treated.
Examples
The present invention will be described in more detail below with reference to examples. It should be noted that the present invention is not limited to the contents of the following examples.
The evaluation methods of physical properties and the like are shown in the following examples.
[ transmittance (%) ]
The average light transmittance of the polyimide film (50 mm. times.50 mm) at 440nm to 780nm was determined by a U4000 type spectrophotometer.
[ glass transition temperature (Tg) ]
The glass transition temperature was determined as follows: the maximum value of the loss tangent (Tan. delta.) was determined from the maximum value of the loss tangent at the time of heating from room temperature to 400 ℃ at a rate of 10 ℃ per minute by using a 10mm wide sample using a viscoelasticity analyzer (RSA-II, Rheometric Scientific F.E.).
[ Coefficient of Thermal Expansion (CTE) ]
A tensile test was conducted at a constant temperature rise rate (20 ℃/min) in a temperature range of 30 ℃ to 260 ℃ while applying a load of 5.0g to a polyimide film having a size of 3mm × 15mm using a thermomechanical analysis (TMA) apparatus, and the thermal expansion coefficient (× 10-6/K)。
[ example 1]
A resin solution of polyamic acid obtained from PDA (1, 4-phenylenediamine) and BPDA (3,3 ', 4, 4' -biphenyltetracarboxylic dianhydride) was coated on a glass substrate as a support so that the thickness after curing was 20 μm and the coating area was 300 mm. times.380 mm, and dried by heating at 130 ℃ to remove the solvent (DMAc: N, N-dimethylacetamide) in the resin solution. Then, imidization was performed by heat treatment at a temperature rise rate of about 1 ℃/min from 160 ℃ to 360 ℃ to form a first polyimide layer having a thickness of 20 μm (surface roughness Ra 1.3nm, Tg 355 ℃).
A resin solution of polyamic acid obtained from PMDA (pyromellitic dianhydride), 6FDA (2,2 ' -bis (3, 4-dicarboxyphenyl) hexafluoropropane dianhydride) and TFMB (2,2 ' -bis (trifluoromethyl) -4,4 ' -diaminobiphenyl) was coated on the first polyimide layer in such a manner that the coating area was larger than that of the first polyimide layer, the entire first polyimide layer was covered with the resin solution, the coating area was 310mm × 390mm, and the thickness after curing was 25 μm, and the solvent (DMAc: N, N-dimethylacetamide) in the resin solution was removed by heating and drying at 130 ℃. Next, imidization was performed by heat treatment at a temperature rise rate of about 20 ℃/min from 160 ℃ to 360 ℃ to form a second polyimide layer having a thickness of 25 μm. The high temperature holding time at this time was 1 minute. In the synthesis of the polyamic acid, the diamine component and the acid dianhydride component were approximately equimolar, and the ratio PMDA/6FDA was 85/15.
This makes a laminate in which a first and a second polyimide layers are laminated in this order on glass, and an EL element serving as a display portion is formed on the second polyimide layer side of the laminate. Then, a notch was cut in the second polyimide layer so as to surround the display portion, and separation was performed at the interface between the first polyimide layer and the second polyimide layer, thereby obtaining a display device having an EL element on a polyimide substrate made of the second polyimide layer. In this case, the first polyimide layer and the second polyimide layer can be easily separated from each other by artificially peeling the layers without using a method such as laser peeling, without damaging devices of a display portion such as a TFT and an electrode. The peel strength of the first polyimide layer and the second polyimide layer was 3.5N/m. In the above examples, the linear expansion coefficient of the first polyimide layer was 12.0ppm/K, and the linear expansion coefficient of the second polyimide layer was 9.7 ppm/K. The transmittance of the second polyimide layer in the wavelength region of 440nm to 780nm was 83.5%.
[ example 2]
A resin solution of polyamic acid obtained from PDA (1, 4-phenylenediamine) and BPDA (3,3 ', 4, 4' -biphenyltetracarboxylic dianhydride) was coated on a glass substrate as a support so that the thickness after curing was 20 μm and the coating area was 310 mm. times.390 mm, and the solvent (DMAc: N, N-dimethylacetamide) in the resin solution was removed by heating and drying at 120 ℃. Then, imidization was performed by heat treatment at a temperature rise rate of about 1 ℃/min from 130 ℃ to 360 ℃ to form a first polyimide layer having a thickness of 25 μm (surface roughness Ra 1.3nm, Tg 355 ℃).
A resin solution of polyamic acid obtained from PMDA (pyromellitic dianhydride), 6FDA (2,2 ' -bis (3, 4-dicarboxyphenyl) hexafluoropropane dianhydride) and TFMB (2,2 ' -bis (trifluoromethyl) -4,4 ' -diaminobiphenyl) was coated on the first polyimide layer so that the coating area was 310mm × 390mm and the thickness after curing was 5 μm, and the solvent (DMAc: N, N-dimethylacetamide) in the resin solution was removed by heating and drying at 130 ℃. Next, imidization was performed by heat treatment at a temperature rise rate of about 20 ℃/min from 160 ℃ to 360 ℃ to form a second polyimide layer having a thickness of 5 μm. In the synthesis of the polyamic acid, the diamine component and the acid dianhydride component were approximately equimolar, and the ratio PMDA/6FDA was 60/40.
This makes a laminate in which a first and a second polyimide layers are laminated in this order on glass, and an EL element serving as a display portion is formed on the second polyimide layer side of the laminate. Then, a notch was cut in the thickness direction of the first polyimide layer and the second polyimide layer so as to surround the display portion, and after removing the glass on the side of the first polyimide layer, the first polyimide layer and the second polyimide layer were peeled off from each other at the interface, thereby obtaining a display device having an EL element on a polyimide substrate made of the second polyimide layer. In this case, the separation can be easily performed without performing artificial peeling such as laser peeling between the glass and the first polyimide layer and between the first polyimide layer and the second polyimide layer without damaging devices of a display portion such as a TFT and an electrode. The peel strength of the first polyimide layer and the second polyimide layer was 4.0N/m. In the above examples, the linear expansion coefficient of the first polyimide layer was 7.0ppm/K, and the linear expansion coefficient of the second polyimide layer was 20.4 ppm/K. The transmittance of the second polyimide layer in the wavelength region of 440 to 780nm was 86.7%.
(example 3)
In order to reuse the laminate of the support and the first polyimide layer separated from the second polyimide layer in example 1, the remaining periphery of the second polyimide layer was removed, and then the laminate was washed with pure water, and further heat-treated at 100 ℃, 200 ℃, 300 ℃, and 360 ℃ for 2 minutes.
On the first polyimide layer, a polyamic acid resin solution was applied in the same manner as in the second polyimide layer of example 1, and the resultant was dried by heating at 130 ℃, and then heated at a rate of about 20 ℃/min from 160 ℃ to 360 ℃ and held at 360 ℃ for 60 minutes to form a second polyimide layer having a thickness of 25 μm. The high temperature holding time at this time was 61 minutes.
Thus, a laminate in which the first polyimide layer and the second polyimide layer were sequentially laminated on the glass was produced, and a display device was obtained in the same manner as in example 1. The peel strength of the first polyimide layer and the second polyimide layer was 10.0N/m, and the layers could be easily separated by a human hand. The linear expansion coefficient of the second polyimide layer was 9.3ppm/K, and the transmittance of the second polyimide layer in the wavelength region of 440 to 780nm was 78.5%.
(example 4)
A resin solution of polyamic acid obtained from 17.70g of m-TB (2,2 ' -dimethylbenzidine), 4.3g of TPE-R (1, 3-bis (4-aminophenoxy) benzene, 17.20g of PMDA (pyromellitic dianhydride), and 5.8g of BPDA (3,3 ', 4,4 ' -biphenyltetracarboxylic dianhydride) was coated on a glass substrate as a support so that the cured thickness was 25 μm and the coating area was 310mm × 390mm, and then dried by heating at 120 ℃ to remove the solvent (DMAc: N, N-dimethylacetamide) in the resin solution, and then imidized by heat treatment at a temperature rise rate of about 15 ℃/min from 130 ℃ to 160 ℃ to form a first polyimide layer having a thickness of 25 μm (surface roughness Ra ═ 1.0nm, Tg ═ 360 ℃).
On the first polyimide layer, a polyamic acid resin solution was applied so that the application area was 306mm × 386mm, and heat-dried at 130 ℃ in the same manner as in the second polyimide layer of example 1, and then, the temperature was raised at a rate of about 20 ℃/min from 160 ℃ to 360 ℃ and held at 360 ℃ for 30 minutes, thereby forming a second polyimide layer having a thickness of 25 μm. The high temperature holding time at this time was 31 minutes.
Thus, a laminate in which the first polyimide layer and the second polyimide layer were sequentially laminated on the glass was produced, and a display device was obtained in the same manner as in example 2. The peel strength of the first polyimide layer and the second polyimide layer was 110N/m, and the layers could be separated by a human hand. The linear expansion coefficient of the first polyimide layer was 20.0ppm/K, and the linear expansion coefficient of the second polyimide layer was 9.5 ppm/K. The transmittance of the second polyimide layer in the wavelength region of 440nm to 780nm was 80.5%.
(example 5)
A resin solution of polyamic acid obtained from PDA (1, 4-phenylenediamine) and BPDA (3,3 ', 4, 4' -biphenyltetracarboxylic dianhydride) was coated on a copper foil so that the cured thickness was 20 μm, and the resin solution was dried by heating at 130 ℃ to remove the solvent (DMAc: N, N-dimethylacetamide). Then, imidization was performed by heat treatment at a temperature rise rate of about 1 ℃/min from 160 ℃ to 360 ℃ to form a first polyimide layer having a thickness of 20 μm (surface roughness Ra 1.3nm, Tg 355 ℃) on the copper foil.
A resin solution of polyamic acid obtained from PMDA (pyromellitic dianhydride), 6FDA (2,2 ' -bis (3, 4-dicarboxyphenyl) hexafluoropropane dianhydride) and TFMB (2,2 ' -bis (trifluoromethyl) -4,4 ' -diaminobiphenyl) was coated on the first polyimide layer so that the thickness after curing was 25 μm, and dried by heating at 130 ℃ to remove the solvent (DMAc: N, N-dimethylacetamide) in the resin solution. Next, imidization was performed by heat treatment at a temperature rise rate of about 20 ℃/min from 160 ℃ to 360 ℃ to form a second polyimide layer having a thickness of 25 μm. In the synthesis of the polyamic acid, the diamine component and the acid dianhydride component were approximately equimolar, and the ratio PMDA/6FDA was 85/15.
The copper foil portion of the laminate composed of copper foil/first polyimide layer/second polyimide layer was removed by ferric chloride etching to obtain a laminate composed of first polyimide layer/second polyimide layer.
The laminated film is bonded to a glass substrate as a support with an epoxy resin adhesive, and then an EL element as a display portion is formed on the second polyimide layer side. Thereafter, the interface between the first polyimide layer and the second polyimide layer was separated by peeling, and a display device having an EL element on a polyimide substrate was obtained. The first polyimide layer and the second polyimide layer can be easily separated without causing damage to devices of a display portion such as a TFT and an electrode. In the above examples, the linear expansion coefficient of the first polyimide layer was 12.0ppm/K, and the linear expansion coefficient of the second polyimide layer was 9.7 ppm/K. The transmittance of the second polyimide layer in the wavelength region of 440nm to 780nm was 83.5%.
Description of the symbols
1 glass substrate
2 peeling off layer
3 polyimide layer
4 display part (TFT/organic EL panel part)
5 cutting line
6 adhesive layer
7 first polyimide layer
8 second polyimide layer
9 cutting area
10 cut surface
Claims (17)
1. A method for manufacturing a display device, characterized in that a predetermined display portion is formed on a second polyimide layer in a state where the first polyimide layer and the second polyimide layer are laminated on a support, and thereafter, a display device having a display portion on a polyimide substrate composed of the second polyimide layer is obtained by separating a boundary surface between the first polyimide layer and a second resin layer,
the peel strength of the first polyimide layer and the second polyimide layer is 200N/m or less,
at least one of the first polyimide layer and the second polyimide layer is composed of a polyimide having a structural unit represented by the following general formula (1),
in the formula, Ar1Represents an organic group having a valence of 4 of an aromatic ring, Ar2Is a 2-valent organic group represented by the following general formula (2) or (3),
wherein R in the general formula (2) or the general formula (3)1～R8Each independently represents a hydrogen atom, a fluorine atom, an alkyl group or alkoxy group having 1 to 5 carbon atoms, or a fluorine-substituted hydrocarbon group, R in the general formula (2)1～R4At least 1 of (a) and R of the formula (3)1～R8At least 1 of them is a fluorine atom or a fluorine-substituted hydrocarbon group.
2. A method for manufacturing a display device, characterized in that a predetermined display portion is formed on a second polyimide layer in a state where the first polyimide layer and the second polyimide layer are laminated on a support, and thereafter, a display device having a display portion on a polyimide substrate composed of the second polyimide layer is obtained by separating a boundary surface between the first polyimide layer and a second resin layer,
the peel strength of the first polyimide layer and the second polyimide layer is 200N/m or less,
at least one of the first polyimide layer and the second polyimide layer is composed of a polyimide having a structural unit represented by the following general formula (1),
in the formula, Ar1Represents 1 or more kinds of 4-valent organic groups selected from the following formulae as acid anhydride residues, Ar2Is an organic radical having a valence of 2, Ar, as a diamine residue1、Ar2Wherein either one of them is an aromatic residue,
3. a method for manufacturing a display device, characterized in that a predetermined display portion is formed on a second polyimide layer in a state where the first polyimide layer and the second polyimide layer are laminated on a support, and thereafter, a display device having a display portion on a polyimide substrate composed of the second polyimide layer is obtained by separating a boundary surface between the first polyimide layer and a second resin layer,
the peel strength of the first polyimide layer and the second polyimide layer is 200N/m or less,
at least one of the first polyimide layer and the second polyimide layer is composed of a polyimide having a structural unit represented by the following general formula (1), and the acid anhydride as a raw material is 1 or more acid anhydrides selected from the group consisting of 3,3 ', 4, 4' -biphenyltetracarboxylic dianhydride and pyromellitic dianhydride,
in the formula, Ar1Represents an organic group having a valence of 4, Ar, as an acid anhydride residue2Is a 2-valent organic group as a diamine residue.
4. The method of manufacturing a display device according to any one of claims 1 to 3, wherein a polyimide laminated film in which the first polyimide layer and the second polyimide layer are directly laminated is bonded to the support, that is, a first polyimide layer surface of the polyimide laminated film is bonded to one surface of the support via an adhesive layer, and then a predetermined display portion is formed on the laminated film, and thereafter, a separation is performed at a boundary surface between the first polyimide layer and the second polyimide layer, thereby obtaining a display device having a display portion on a polyimide substrate made of the second polyimide layer.
5. The method for manufacturing a display device according to any one of claims 1 to 3, wherein a display device having a display portion on a polyimide substrate is obtained by removing the support after forming a predetermined display portion and then separating a boundary surface between the first polyimide layer and the second polyimide layer.
6. The method for manufacturing a display device according to any one of claims 1 to 3, wherein the formation of the first polyimide layer is performed by laminating polyimide films, and the formation of the second polyimide layer is performed by applying a resin solution of polyimide or a polyimide precursor.
7. The method for manufacturing a display device according to any one of claims 1 to 3, wherein the formation of the first polyimide layer and the second polyimide layer is performed by coating, heating a resin solution of polyimide or a polyimide precursor.
8. The method for manufacturing a display device according to any one of claims 1 to 3, wherein a part of the second polyimide layer protrudes from a peripheral portion of the first polyimide layer, and the protruding portion of the second polyimide layer is fixed to the support.
9. The method for manufacturing a display device according to any one of claims 1 to 3, wherein a part of one of the first polyimide layer and the second polyimide layer protrudes from a peripheral portion of the other layer.
10. The method for manufacturing a display device according to any one of claims 1 to 3, wherein the separation of the first polyimide layer and the second polyimide layer is performed after the first polyimide layer is cut into the slit along the outer periphery of the display portion.
11. The method for manufacturing a display device according to any one of claims 1 to 3, wherein when the formation of the second polyimide layer is performed by heating after coating the resin solution of polyimide or a polyimide precursor, a high-temperature retention time of the second polyimide layer is less than 60 minutes.
12. The method for manufacturing a display device according to any one of claims 1 to 3, wherein the support is a glass substrate.
13. The method for manufacturing a display device according to any one of claims 1 to 3, wherein the first polyimide layer has a thermal expansion coefficient of 25ppm/K or less.
14. The method for manufacturing a display device according to any one of claims 1 to 3, wherein the second polyimide layer has a thermal expansion coefficient of 25ppm/K or less.
15. The method for manufacturing a display device according to any one of claims 1 to 3, wherein the second polyimide layer has a transmittance of 80% or more in a wavelength region of 440nm to 780 nm.
16. The method for manufacturing a display device according to any one of claims 1 to 3, wherein the display portion is formed with a gas barrier layer interposed therebetween, and a difference in thermal expansion coefficient between the second polyimide layer and the gas barrier layer is 10ppm/K or less.
17. The method for manufacturing a display device according to any one of claims 1 to 3, wherein the display portion is a color filter layer.
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| KR101773651B1 (en) * | 2013-04-09 | 2017-08-31 | 주식회사 엘지화학 | Laminate structure for manufacturing substrate and device comprising substrate manufactured by using same |
| WO2015012339A1 (en) * | 2013-07-24 | 2015-01-29 | ユニチカ株式会社 | Laminate, method for processing same, and method for manufacturing flexible device |
| KR102340689B1 (en) * | 2014-03-31 | 2021-12-16 | 닛산 가가쿠 가부시키가이샤 | Composition for forming releasing layer |
| JP6473931B2 (en) | 2014-05-29 | 2019-02-27 | パナソニックＩｐマネジメント株式会社 | Resin substrate with support substrate, manufacturing method thereof, and electronic device using the resin substrate |
| KR102352849B1 (en) * | 2014-12-23 | 2022-01-18 | 엘지디스플레이 주식회사 | Method for manufacturing flexible display and flexible display |
| JP6503183B2 (en) * | 2014-12-24 | 2019-04-17 | 株式会社カネカ | Polyimide laminate, electronic device, and method of manufacturing electronic device |
| CN113402882B (en) * | 2015-02-10 | 2024-02-06 | 日产化学工业株式会社 | Composition for forming release layer |
| KR102656566B1 (en) * | 2015-03-26 | 2024-04-12 | 도레이 카부시키가이샤 | Resin laminated film, laminated body containing the same, TFT substrate, organic EL device color filter, and method for manufacturing the same |
| CN107960094B (en) * | 2015-03-31 | 2021-03-12 | 日产化学工业株式会社 | Composition for forming release layer and release layer |
| JP6808401B2 (en) * | 2015-08-31 | 2021-01-06 | 日鉄ケミカル＆マテリアル株式会社 | Manufacturing method of polyimide substrate film with functional layer |
| JP6706475B2 (en) * | 2015-09-30 | 2020-06-10 | 日鉄ケミカル＆マテリアル株式会社 | Long polyimide laminate film and method for producing the same, and method for producing polyimide film with functional layer |
| JP6937557B2 (en) * | 2015-09-30 | 2021-09-22 | 日鉄ケミカル＆マテリアル株式会社 | Method of manufacturing polyimide film |
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| TW201425048A (en) | 2014-07-01 |
| JP6284562B2 (en) | 2018-02-28 |
| KR20150060716A (en) | 2015-06-03 |
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| KR20200026322A (en) | 2020-03-10 |
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| JP5898328B2 (en) | 2016-04-06 |
| KR102094729B1 (en) | 2020-03-30 |
| JP2016145987A (en) | 2016-08-12 |
| CN107728358A (en) | 2018-02-23 |
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