TW202103913A - Laminated substrate and bundled body which has a polyimide resin layer laminated on a supporting substrate made of glass, and a protective film covering the polyimide resin layer - Google Patents

Laminated substrate and bundled body which has a polyimide resin layer laminated on a supporting substrate made of glass, and a protective film covering the polyimide resin layer Download PDF

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TW202103913A
TW202103913A TW109117780A TW109117780A TW202103913A TW 202103913 A TW202103913 A TW 202103913A TW 109117780 A TW109117780 A TW 109117780A TW 109117780 A TW109117780 A TW 109117780A TW 202103913 A TW202103913 A TW 202103913A
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resin layer
protective film
polyimide resin
substrate
laminated
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TW109117780A
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Chinese (zh)
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TWI803752B (en
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長尾洋平
川崎周馬
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日商Ａｇｃ股份有限公司
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    • 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
    • B32B17/00—Layered products essentially comprising sheet glass, or glass, slag, or like fibres
    • B32B17/06—Layered products essentially comprising sheet glass, or glass, slag, or like fibres comprising glass as the main or only constituent of a layer, next to another layer of a specific material
    • B32B17/10—Layered products essentially comprising sheet glass, or glass, slag, or like fibres comprising glass as the main or only constituent of a layer, next to another layer of a specific material of synthetic resin
    • 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
    • B32B17/00—Layered products essentially comprising sheet glass, or glass, slag, or like fibres
    • B32B17/06—Layered products essentially comprising sheet glass, or glass, slag, or like fibres comprising glass as the main or only constituent of a layer, next to another layer of a specific material
    • B32B17/10—Layered products essentially comprising sheet glass, or glass, slag, or like fibres comprising glass as the main or only constituent of a layer, next to another layer of a specific material of synthetic resin
    • B32B17/10005—Layered products essentially comprising sheet glass, or glass, slag, or like fibres comprising glass as the main or only constituent of a layer, next to another layer of a specific material of synthetic resin laminated safety glass or glazing
    • B32B17/10009—Layered products essentially comprising sheet glass, or glass, slag, or like fibres comprising glass as the main or only constituent of a layer, next to another layer of a specific material of synthetic resin laminated safety glass or glazing characterized by the number, the constitution or treatment of glass sheets
    • B32B17/10018—Layered products essentially comprising sheet glass, or glass, slag, or like fibres comprising glass as the main or only constituent of a layer, next to another layer of a specific material of synthetic resin laminated safety glass or glazing characterized by the number, the constitution or treatment of glass sheets comprising only one glass sheet
    • 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
    • B32B27/06—Layered products comprising a layer of synthetic resin as the main or only constituent of a layer, which is next to another layer of the same or of a different material
    • B32B27/08—Layered products comprising a layer of synthetic resin as the main or only constituent of a layer, which is next to another layer of the same or of a different material of synthetic resin
    • 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
    • B32B27/28—Layered products comprising a layer of synthetic resin comprising synthetic resins not wholly covered by any one of the sub-groups B32B27/30 - B32B27/42
    • B32B27/281—Layered products comprising a layer of synthetic resin comprising synthetic resins not wholly covered by any one of the sub-groups B32B27/30 - B32B27/42 comprising polyimides
    • 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
    • B32B27/28—Layered products comprising a layer of synthetic resin comprising synthetic resins not wholly covered by any one of the sub-groups B32B27/30 - B32B27/42
    • B32B27/283—Layered products comprising a layer of synthetic resin comprising synthetic resins not wholly covered by any one of the sub-groups B32B27/30 - B32B27/42 comprising polysiloxanes
    • 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
    • B32B27/32—Layered products comprising a layer of synthetic resin comprising polyolefins
    • 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
    • B32B3/00—Layered products comprising a layer with external or internal discontinuities or unevennesses, or a layer of non-planar shape; Layered products comprising a layer having particular features of form
    • B32B3/02—Layered products comprising a layer with external or internal discontinuities or unevennesses, or a layer of non-planar shape; Layered products comprising a layer having particular features of form characterised by features of form at particular places, e.g. in edge regions
    • B32B3/08—Layered products comprising a layer with external or internal discontinuities or unevennesses, or a layer of non-planar shape; Layered products comprising a layer having particular features of form characterised by features of form at particular places, e.g. in edge regions characterised by added members at particular parts
    • 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
    • B32B7/00—Layered products characterised by the relation between layers; Layered products characterised by the relative orientation of features between layers, or by the relative values of a measurable parameter between layers, i.e. products comprising layers having different physical, chemical or physicochemical properties; Layered products characterised by the interconnection of layers
    • B32B7/04—Interconnection of layers
    • B32B7/06—Interconnection of layers permitting easy separation
    • 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
    • B32B7/00—Layered products characterised by the relation between layers; Layered products characterised by the relative orientation of features between layers, or by the relative values of a measurable parameter between layers, i.e. products comprising layers having different physical, chemical or physicochemical properties; Layered products characterised by the interconnection of layers
    • B32B7/04—Interconnection of layers
    • B32B7/12—Interconnection of layers using interposed adhesives or interposed materials with bonding properties
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B65—CONVEYING; PACKING; STORING; HANDLING THIN OR FILAMENTARY MATERIAL
    • B65D—CONTAINERS FOR STORAGE OR TRANSPORT OF ARTICLES OR MATERIALS, e.g. BAGS, BARRELS, BOTTLES, BOXES, CANS, CARTONS, CRATES, DRUMS, JARS, TANKS, HOPPERS, FORWARDING CONTAINERS; ACCESSORIES, CLOSURES, OR FITTINGS THEREFOR; PACKAGING ELEMENTS; PACKAGES
    • B65D71/00—Bundles of articles held together by packaging elements for convenience of storage or transport, e.g. portable segregating carrier for plural receptacles such as beer cans or pop bottles; Bales of material
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
    • H01L21/00—Processes or apparatus adapted for the manufacture or treatment of semiconductor or solid state devices or of parts thereof
    • H01L21/67—Apparatus specially adapted for handling semiconductor or electric solid state devices during manufacture or treatment thereof; Apparatus specially adapted for handling wafers during manufacture or treatment of semiconductor or electric solid state devices or components ; Apparatus not specifically provided for elsewhere
    • H01L21/683—Apparatus specially adapted for handling semiconductor or electric solid state devices during manufacture or treatment thereof; Apparatus specially adapted for handling wafers during manufacture or treatment of semiconductor or electric solid state devices or components ; Apparatus not specifically provided for elsewhere for supporting or gripping
    • H01L21/6835—Apparatus specially adapted for handling semiconductor or electric solid state devices during manufacture or treatment thereof; Apparatus specially adapted for handling wafers during manufacture or treatment of semiconductor or electric solid state devices or components ; Apparatus not specifically provided for elsewhere for supporting or gripping using temporarily an auxiliary support
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
    • H01L23/00—Details of semiconductor or other solid state devices
    • H01L23/12—Mountings, e.g. non-detachable insulating substrates
    • H01L23/14—Mountings, e.g. non-detachable insulating substrates characterised by the material or its electrical properties
    • H01L23/145—Organic substrates, e.g. plastic
    • 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
    • B32B2255/00—Coating on the layer surface
    • B32B2255/10—Coating on the layer surface on synthetic resin layer or on natural or synthetic rubber layer
    • 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
    • B32B2255/00—Coating on the layer surface
    • B32B2255/26—Polymeric coating
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
    • H01L2221/00—Processes or apparatus adapted for the manufacture or treatment of semiconductor or solid state devices or of parts thereof covered by H01L21/00
    • H01L2221/67—Apparatus for handling semiconductor or electric solid state devices during manufacture or treatment thereof; Apparatus for handling wafers during manufacture or treatment of semiconductor or electric solid state devices or components; Apparatus not specifically provided for elsewhere
    • H01L2221/683—Apparatus for handling semiconductor or electric solid state devices during manufacture or treatment thereof; Apparatus for handling wafers during manufacture or treatment of semiconductor or electric solid state devices or components; Apparatus not specifically provided for elsewhere for supporting or gripping
    • H01L2221/68304—Apparatus for handling semiconductor or electric solid state devices during manufacture or treatment thereof; Apparatus for handling wafers during manufacture or treatment of semiconductor or electric solid state devices or components; Apparatus not specifically provided for elsewhere for supporting or gripping using temporarily an auxiliary support
    • H01L2221/68377—Apparatus for handling semiconductor or electric solid state devices during manufacture or treatment thereof; Apparatus for handling wafers during manufacture or treatment of semiconductor or electric solid state devices or components; Apparatus not specifically provided for elsewhere for supporting or gripping using temporarily an auxiliary support with parts of the auxiliary support remaining in the finished device

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  • Engineering & Computer Science (AREA)
  • Physics & Mathematics (AREA)
  • Condensed Matter Physics & Semiconductors (AREA)
  • General Physics & Mathematics (AREA)
  • Computer Hardware Design (AREA)
  • Microelectronics & Electronic Packaging (AREA)
  • Power Engineering (AREA)
  • Mechanical Engineering (AREA)
  • Manufacturing & Machinery (AREA)
  • Laminated Bodies (AREA)
  • Buffer Packaging (AREA)
  • Packaging Frangible Articles (AREA)

Abstract

The present invention relates to a laminated substrate which has a polyimide resin layer laminated on a supporting substrate made of glass, and a protective film covering the polyimide resin layer. When the first adhesion force between the polyimide resin layer and the protective film is F1 and the second adhesion force between the supporting substrate and the protective film is F2, the first adhesion force F1 is 0.001 N/10 mm ≤ F1 ≤ 0.17 N/10 mm and the above-mentioned second adhesion force F2 is 0.05 N/10 mm ≤ F2 ≤ (F1(N/10 mm)+0.3 N/10 mm).

Description

積層基板及捆包體Laminated substrate and package

本發明係關於一種積層基板及捆包體。The present invention relates to a laminated substrate and package body.

製造如太陽能電池；液晶面板(LCD，Liquid Crystal Display)；有機EL面板(OLED，OrganicLight-Emitting Diode)；感測電磁波、X射線、紫外線、可見光線、紅外線等之接收感測器面板；等電子裝置時，如專利文獻1所記載，揭示有一種使用聚醯亞胺樹脂層作為基板之態樣。聚醯亞胺樹脂層以設置於玻璃基板上之積層基板之狀態使用，並將積層基板提供於製造電子裝置。形成電子裝置後，將聚醯亞胺樹脂層與玻璃基板分離。Manufacturing such as solar cells; liquid crystal panels (LCD, Liquid Crystal Display); organic EL panels (OLED, Organic Light-Emitting Diode); receiving sensor panels for sensing electromagnetic waves, X-rays, ultraviolet rays, visible rays, infrared rays, etc.; and other electronics In the case of a device, as described in Patent Document 1, there is disclosed an aspect in which a polyimide resin layer is used as a substrate. The polyimide resin layer is used in the state of a build-up substrate provided on a glass substrate, and the build-up substrate is provided for manufacturing electronic devices. After the electronic device is formed, the polyimide resin layer is separated from the glass substrate.

另一方面，搬送複數片玻璃基板時，例如如專利文獻2所記載，以介隔包含原紙漿之襯紙積層複數片玻璃板而成之玻璃板捆包體之形式搬送。 [先前技術文獻] [專利文獻]On the other hand, when conveying a plurality of glass substrates, for example, as described in Patent Document 2, it is conveyed in the form of a glass plate package in which a plurality of glass plates are laminated via a backing paper containing base pulp. [Prior Technical Literature] [Patent Literature]

[專利文獻1]日本專利特開2015-104843號公報 [專利文獻2]日本國內公開第2016/104450號[Patent Document 1] Japanese Patent Laid-Open No. 2015-104843 [Patent Document 2] Japan Domestic Publication No. 2016/104450

[發明所欲解決之問題][The problem to be solved by the invention]

如上所述，為了於積層基板中之聚醯亞胺樹脂層上，形成構成電子裝置之各種電子裝置用構件，期望聚醯亞胺樹脂層之表面無損傷或異物。 另一方面，本發明者等人發現雖如專利文獻2所記載，嘗試使用介隔包含原紙漿之襯紙，積層複數片於玻璃基板上形成聚醯亞胺樹脂層而成之積層基板所得之捆包體，搬送複數片積層基板，但於重疊之積層基板中之聚醯亞胺樹脂層之表面產生了損傷。 又，本發明者等人發現，雖嘗試取代襯紙，將保護膜貼合於聚醯亞胺樹脂層以防止產生上述損傷，但根據保護膜之種類，有剝離保護膜時，支持基材破損之情形、或剝離保護膜後，於聚醯亞胺樹脂層表面上產生異物之情形、或於聚醯亞胺樹脂層之外周部分產生異物之情形。 因此，本發明之目的在於提供一種積層時亦抑制於聚醯亞胺樹脂層之表面產生損傷，剝離保護膜時，抑制支持基材之破損，再者，抑制聚醯亞胺樹脂層上之異物產生的積層基板，及裝載有複數片積層基板之捆包體。 [解決問題之技術手段]As described above, in order to form various electronic device components constituting the electronic device on the polyimide resin layer in the laminated substrate, it is desirable that the surface of the polyimide resin layer is free of damage or foreign matter. On the other hand, the inventors of the present invention found that although as described in Patent Document 2, they tried to use a backing paper containing base pulp, and laminated a plurality of sheets on a glass substrate to form a polyimide resin layer. The packaged body conveyed a plurality of laminated substrates, but the surface of the polyimide resin layer in the laminated laminated substrates was damaged. In addition, the inventors of the present invention have discovered that, although trying to replace the backing paper and attach a protective film to the polyimide resin layer to prevent the above-mentioned damage, depending on the type of the protective film, when the protective film is peeled off, the supporting substrate is damaged. In this case, or after the protective film is peeled off, foreign matter is generated on the surface of the polyimide resin layer, or foreign matter is generated on the outer periphery of the polyimide resin layer. Therefore, the object of the present invention is to provide a method for suppressing damage to the surface of the polyimide resin layer during lamination, suppressing damage to the supporting substrate when the protective film is peeled off, and further suppressing foreign matter on the polyimide resin layer The generated laminated substrate and the package body loaded with a plurality of laminated substrates. [Technical means to solve the problem]

本發明者等人進行積極研討，結果發現可藉由以下構成達成上述目的。 本發明之第1態樣係提供一種積層基板，其係於玻璃製之支持基材上，積層有聚醯亞胺樹脂層、與覆蓋聚醯亞胺樹脂層之保護膜者，且將聚醯亞胺樹脂層與保護膜之第1密著力設為F1 ，將支持基材與保護膜之第2密著力設為F2 時，第1密著力F1 為0.001 N/10 mm≦F1 ≦0.17 N/10 mm，第2密著力F2 為0.05 N/10 mm≦F2 ≦(F1 (N/10 mm)+0.3 N/10 mm)。 較佳為保護膜之大小為支持基材之大小以上。 較佳為保護膜之厚度為20 μm以上。 較佳為保護膜具有基材、及積層於基材，且與聚醯亞胺樹脂層相接之密著層，基材由聚乙烯構成。 較佳為支持基材與聚醯亞胺樹脂層之密著力大於第1密著力及第2密著力之任一者。 較佳為於支持基材與聚醯亞胺樹脂層間，設置有矽烷偶合劑層。 較佳為於支持基材與聚醯亞胺樹脂層間，設置有矽酮樹脂層。 本發明之第2態樣提供一種捆包體，其具有托板、及於托板裝載複數片之上述第1態樣之積層基板。 較佳為複數片積層基板以相互施加荷重之狀態裝載於托板。 較佳為托板具有底板、及立設於底板之背板，且積層基板以使支持基材朝向背板之表面傾斜之狀態裝載於托板。 較佳為積層基板之大小係短邊為850 mm以上，長邊為1100 mm以上。 [發明之效果]The inventors of the present invention conducted active studies and found that the above-mentioned object can be achieved by the following configuration. The first aspect of the present invention provides a laminated substrate, which is on a supporting substrate made of glass, laminated with a polyimide resin layer, and a protective film covering the polyimide resin layer, and the polyimide resin layer When the first adhesion force between the imine resin layer and the protective film is F 1 , and the second adhesion force between the support base material and the protective film is F 2 , the first adhesion force F 1 is 0.001 N/10 mm≦F 1 ≦0.17 N/10 mm, the second adhesion force F 2 is 0.05 N/10 mm≦F 2 ≦(F 1 (N/10 mm)+0.3 N/10 mm). Preferably, the size of the protective film is greater than the size of the supporting substrate. Preferably, the thickness of the protective film is 20 μm or more. Preferably, the protective film has a base material and an adhesion layer laminated on the base material and in contact with the polyimide resin layer, and the base material is made of polyethylene. Preferably, the adhesion force between the support substrate and the polyimide resin layer is greater than any one of the first adhesion force and the second adhesion force. Preferably, a silane coupling agent layer is provided between the supporting substrate and the polyimide resin layer. Preferably, a silicone resin layer is provided between the supporting substrate and the polyimide resin layer. A second aspect of the present invention provides a package having a pallet, and a plurality of laminated substrates of the above-mentioned first aspect are mounted on the pallet. Preferably, a plurality of laminated substrates are mounted on the pallet in a state where a load is applied to each other. Preferably, the pallet has a bottom plate and a back plate standing on the bottom plate, and the laminated substrate is loaded on the pallet in a state where the supporting base material is inclined toward the surface of the back plate. Preferably, the size of the laminated substrate is 850 mm or more on the short side and 1100 mm or more on the long side. [Effects of Invention]

根據本發明，提供一種抑制積層時亦於聚醯亞胺樹脂之表面產生損傷，抑制剝離保護膜時支持基材之破損，進而抑制聚醯亞胺樹脂層上之異物產生之積層基板，及載置有複數個積層基板之捆包體。According to the present invention, there is provided a laminated substrate that suppresses damage to the surface of the polyimide resin during lamination, suppresses the breakage of the support base material when the protective film is peeled off, and further suppresses the generation of foreign matter on the polyimide resin layer, and a carrier A package containing a plurality of laminated substrates.

以下，參照圖式，針對本發明之實施形態進行說明。但，以下之實施形態係用以說明本發明之例示者，本發明不限制於以下所示之實施形態。另，可不脫離本發明之範圍，對以下之實施形態加入各種變化及置換。 使用「~」表示之數值範圍意指將「~」前後所記載之數值作為下限值及上限值包含之範圍。Hereinafter, embodiments of the present invention will be described with reference to the drawings. However, the following embodiments are examples for explaining the present invention, and the present invention is not limited to the embodiments shown below. In addition, various changes and substitutions can be added to the following embodiments without departing from the scope of the present invention. The numerical range indicated by "~" means the range that includes the numerical value before and after "~" as the lower limit and the upper limit.

作為本發明之積層基板之特徵點，可例舉設置有覆蓋聚醯亞胺樹脂層之保護膜之點。尤其藉由調整保護膜與聚醯亞胺樹脂層及支持基材間之密著力，而獲得期望之效果。 本發明者等人發現，使用專利文獻2所記載之包含原紙漿之襯紙時，作為於聚醯亞胺樹脂層表面產生損傷之原因，可例舉襯紙與聚醯亞胺樹脂層間之密著力過低之點。即，由於襯紙與聚醯亞胺樹脂層間之密著力較弱，如於襯紙與聚醯亞胺樹脂層間產生摩擦，而於聚醯亞胺樹脂層之表面產生損傷。另一方面，若聚醯亞胺樹脂層與保護膜之密著力過強，則剝離保護膜時，來源於保護膜之成分(例如，密著層之材料)之異物殘留於聚醯亞胺樹脂層上。 考慮以上之點，調整保護膜與聚醯亞胺樹脂層間之密著力。 再者，若保護膜與支持基材間之密著力過弱，則容易保護膜剝離，異物附著於聚醯亞胺樹脂層之外周部分。另一方面，若保護膜與支持基材間之密著力過強，則剝離保護膜時，於聚醯亞胺樹脂層部分與支持基材部分間產生剝離速度差，而於剝離保護膜時對支持基材施加不期望之力，致使支持基材之破壞。 考慮以上之點，調整保護膜與支持基材間之密著力。As a characteristic point of the multilayer substrate of the present invention, a point in which a protective film covering the polyimide resin layer is provided can be exemplified. Especially by adjusting the adhesion between the protective film and the polyimide resin layer and the supporting substrate, the desired effect can be obtained. The inventors of the present invention have discovered that when the backing paper containing base pulp described in Patent Document 2 is used, as the cause of the damage on the surface of the polyimide resin layer, the density between the backing paper and the polyimide resin layer can be cited as an example. Focus on the low point. That is, due to the weak adhesion between the liner paper and the polyimide resin layer, friction occurs between the liner paper and the polyimide resin layer, and damage occurs on the surface of the polyimide resin layer. On the other hand, if the adhesion between the polyimide resin layer and the protective film is too strong, when the protective film is peeled off, foreign matter derived from the components of the protective film (for example, the material of the adhesion layer) remains in the polyimide resin Layer up. Considering the above points, adjust the adhesion between the protective film and the polyimide resin layer. Furthermore, if the adhesive force between the protective film and the supporting base material is too weak, the protective film is easily peeled off, and foreign matter adheres to the outer peripheral portion of the polyimide resin layer. On the other hand, if the adhesion between the protective film and the supporting substrate is too strong, when the protective film is peeled off, a difference in the peeling speed will occur between the polyimide resin layer part and the supporting substrate part. The supporting substrate exerts undesirable force, resulting in the destruction of the supporting substrate. Considering the above points, adjust the adhesion between the protective film and the supporting substrate.

＜積層基板＞ [積層基板之第1例] 圖1係模式性顯示本發明之實施形態之積層基板之第1例之俯視圖，圖2係模式性顯示本發明之實施形態之積層基板之第1例之剖視圖。圖3係模式性顯示本發明之實施形態之積層基板之第1例之保護膜之剖視圖。 第1例之積層基板10係於玻璃製之支持基材12上，積層有聚醯亞胺樹脂層14、與覆蓋聚醯亞胺樹脂層14之保護膜16者。 如圖2所示，於支持基材12之表面12a，設置有聚醯亞胺樹脂層14。如圖1所示，聚醯亞胺樹脂層14之面積小於支持基材12之表面12a，而未設置於支持基材12之表面12a全域。於支持基材12之表面12a之外緣部12c，即支持基材12之額緣部分，未設置聚醯亞胺樹脂層14。 保護膜16覆蓋支持基材12上之聚醯亞胺樹脂層14而配置。如圖2及圖3所示，保護膜16具有基材18、與積層於基材18之密著層19。如圖2所示，保護膜16之密著層19與聚醯亞胺樹脂層14之表面14a及支持基材12之表面12a相接。保護膜16於使用聚醯亞胺樹脂層14作為基板時被剝離。該情形時，有時保護膜16之密著層19自與聚醯亞胺樹脂層14之表面14a及支持基材12之表面12a同時相接之狀態被剝離。＜Multilayer substrates＞ [First example of multilayer substrate] FIG. 1 is a plan view schematically showing the first example of the multilayer substrate of the embodiment of the present invention, and FIG. 2 is a cross-sectional view schematically showing the first example of the multilayer substrate of the embodiment of the present invention. Fig. 3 is a cross-sectional view schematically showing the protective film of the first example of the multilayer substrate of the embodiment of the present invention. The laminated substrate 10 of the first example is on a supporting base material 12 made of glass, and a polyimide resin layer 14 and a protective film 16 covering the polyimide resin layer 14 are laminated. As shown in FIG. 2, a polyimide resin layer 14 is provided on the surface 12a of the supporting substrate 12. As shown in FIG. 1, the area of the polyimide resin layer 14 is smaller than the surface 12 a of the support substrate 12, and is not disposed on the entire surface 12 a of the support substrate 12. On the outer edge portion 12c of the surface 12a of the support substrate 12, that is, the front edge portion of the support substrate 12, the polyimide resin layer 14 is not provided. The protective film 16 is configured to cover the polyimide resin layer 14 on the support base 12. As shown in FIGS. 2 and 3, the protective film 16 has a base material 18 and an adhesion layer 19 laminated on the base material 18. As shown in FIG. 2, the adhesion layer 19 of the protective film 16 is in contact with the surface 14 a of the polyimide resin layer 14 and the surface 12 a of the support base 12. The protective film 16 is peeled off when the polyimide resin layer 14 is used as a substrate. In this case, the adhesion layer 19 of the protective film 16 may be peeled from the state in contact with the surface 14a of the polyimide resin layer 14 and the surface 12a of the support base 12 at the same time.

支持基材12為支持聚醯亞胺樹脂層14之構件，且作為補強聚醯亞胺樹脂層14之補強板發揮功能。又，支持基材12亦作為搬送積層基板10時之搬送基板發揮功能。 於積層基板10中，若對剝離支持基材12與聚醯亞胺樹脂層14之方向施加力，則分離成支持基材12與聚醯亞胺樹脂層14。 聚醯亞胺樹脂層14為用以製造電子裝置所用之基板。於聚醯亞胺樹脂層14之表面14a，形成有構成電子裝置之電晶體、線圈及電阻等電子元件以及信號線等。 保護膜16係保護支持基材12及聚醯亞胺樹脂層14者，尤其以不使聚醯亞胺樹脂層14產生起因於自外部受到之力之打痕及損傷等之方式進行保護。保護膜16例如於圖1所示之積層基板10中為與支持基材12相同之大小。The support base 12 is a member that supports the polyimide resin layer 14 and functions as a reinforcing plate for reinforcing the polyimide resin layer 14. In addition, the supporting base 12 also functions as a transport substrate when transporting the build-up substrate 10. In the laminated substrate 10, when a force is applied to the direction in which the support base 12 and the polyimide resin layer 14 are peeled off, the support base 12 and the polyimide resin layer 14 are separated into the support base 12 and the polyimide resin layer 14. The polyimide resin layer 14 is a substrate used for manufacturing electronic devices. On the surface 14a of the polyimide resin layer 14, electronic components such as transistors, coils, resistors, etc., and signal lines that constitute electronic devices are formed. The protective film 16 protects the support base 12 and the polyimide resin layer 14, and in particular protects the polyimide resin layer 14 from scratches and damage caused by external forces. The protective film 16 is, for example, the same size as the supporting base 12 in the laminated substrate 10 shown in FIG. 1.

積層基板10中，將聚醯亞胺樹脂層14與保護膜16之第1密著力設為F1 ，將支持基材12與保護膜16之第2密著力設為F2 時， 第1密著力F1 為0.001 N/10 mm≦F1 ≦0.17 N/10 mm。第2密著力F2 為0.05 N/10 mm≦F2 ≦(F1 (N/10 mm)+0.3 N/10 mm)。 上述第1密著力F1 及第2密著力F2 之測定如下進行。首先，將切成寬度為25 mm之短條狀之保護膜16貼合於聚醯亞胺樹脂層14或支持基材12。接著，於每1cm2 施加16 g荷重之狀態下，於溫度40°C、相對濕度80%之環境下，放置5天。其後，實施90°C剝離試驗。剝離之上提速度設為300 mm/min。根據穩定剝離之區域之荷重，算出剝離每單位寬度(10 mm)之保護膜時之荷重。In the laminated substrate 10, when the first adhesive force between the polyimide resin layer 14 and the protective film 16 is F 1 , and the second adhesive force between the support base 12 and the protective film 16 is F 2 , the first dense The focus force F 1 is 0.001 N/10 mm≦F 1 ≦0.17 N/10 mm. The second adhesion force F 2 is 0.05 N/10 mm≦F 2 ≦(F 1 (N/10 mm)+0.3 N/10 mm). The measurement of the first adhesion force F 1 and the second adhesion force F 2 is performed as follows. First, the protective film 16 cut into a short strip with a width of 25 mm is attached to the polyimide resin layer 14 or the supporting substrate 12. Then, under the condition of applying a load of 16 g per 1 cm 2, leave it for 5 days in an environment with a temperature of 40°C and a relative humidity of 80%. Thereafter, a 90°C peel test was implemented. The peeling and lifting speed is set to 300 mm/min. Calculate the load when peeling off the protective film per unit width (10 mm) based on the load of the stable peeling area.

如上所述，第1密著力F1 為0.001 N/10 mm≦F1 ≦0.17 N/10 mm。第1密著力F1 未達0.001 N/10 mm時，聚醯亞胺樹脂層14與保護膜16未充分密著，而於聚醯亞胺樹脂層14與保護膜16間產生摩擦，於聚醯亞胺樹脂層14之表面14a產生損傷。 若第1密著力F1 超出0.17 N/10 mm，則聚醯亞胺樹脂層14與保護膜16之密著力過強，保護膜16之密著層19之一部分殘留於聚醯亞胺樹脂層14之表面14a，致使異物產生。尤其，於密著層為包含黏著剤之黏著層之情形時，產生來源於黏著剤之黏著剤殘留。另，若產生異物(尤其黏著剤殘留)，則有聚醯亞胺樹脂層14之耐熱性降低、或有時於使用聚醯亞胺樹脂層14形成之電子裝置中產生斷線等之缺陷。再者，如第1密著力F1 超出1.5 N/10 mm之第1密著力F1 過大之情形時，有產生支持基材12之破壞之情形。 其中，基於進一步抑制聚醯亞胺樹脂層14表面14a產生損傷、及產生異物之點，第1密著力F1 較佳為0.002～0.15 N/10 mm，更佳為0.003～0.145 N/10 mm。As described above, the first adhesion force F 1 is 0.001 N/10 mm≦F 1 ≦0.17 N/10 mm. When the first focus F. 1 adhesion less than 0.001 N / 10 mm, polyimide resin layer 14 and the protective film 16 is not sufficient adhesion, friction is generated between the polyimide in the resin layer 14 and the protective film 16, poly The surface 14a of the imide resin layer 14 is damaged. If the first adhesion force F 1 exceeds 0.17 N/10 mm, the adhesion between the polyimide resin layer 14 and the protective film 16 is too strong, and a part of the adhesion layer 19 of the protective film 16 remains on the polyimide resin layer The surface 14a of 14 causes foreign matter to be generated. In particular, when the adhesive layer is an adhesive layer containing an adhesive, the adhesive residue derived from the adhesive is generated. In addition, if foreign matter (especially residual adhesive) is generated, the heat resistance of the polyimide resin layer 14 may decrease, or defects such as disconnection may occur in the electronic device formed using the polyimide resin layer 14. Furthermore, if the first adhesion force F 1 exceeds 1.5 N/10 mm, the first adhesion force F 1 is too large, the supporting substrate 12 may be damaged. Among them, the first adhesion force F 1 is preferably 0.002 to 0.15 N/10 mm, more preferably 0.003 to 0.145 N/10 mm in order to further suppress the occurrence of damage on the surface 14a of the polyimide resin layer 14 and the generation of foreign matter. .

如上所述，第2密著力F2 為0.05 N/10 mm≦F2 ≦(F1 (N/10 mm)+0.3 N/10 mm)。第2密著力F2 之上限值大於第1密著力F1 。 第2密著力F2 未達0.05 N/10 mm時，保護膜16與支持基材12之密著力過弱，支持基材12之外緣部12c之保護膜16於搬運中捲起，致使異物大量附著於聚醯亞胺樹脂層14之外周部分。藉由該異物，於聚醯亞胺樹脂層14中產生損傷等之可能性提高。 若第2密著力F2 超出F1 (N/10 mm)+0.3 N/10 mm，則保護膜16與支持基材12之密著力過強，剝離保護膜16時，於聚醯亞胺樹脂層14部分與支持基材12部分間產生剝離速度差，而於剝離保護膜16時對支持基材12施加不期望之力，導致支持基材12之破壞。 積層基板10中，由於支持基材12與保護膜16之第2密著力F2 在上述範圍內，故可於剝離保護膜16時順利地剝離，不會產生支持基材12之損傷等。 其中，基於進一步抑制聚醯亞胺樹脂層14之表面14a產生異物、及支持基材12之破損之點，第2密著力F2 較佳為0.06～0.18 N/10 mm，更佳為0.07～0.17 N/10 mm。As described above, the second adhesion force F 2 is 0.05 N/10 mm≦F 2 ≦(F 1 (N/10 mm)+0.3 N/10 mm). The upper limit of the second adhesion force F 2 is greater than the first adhesion force F 1 . When the second adhesion force F 2 is less than 0.05 N/10 mm, the adhesion between the protective film 16 and the supporting substrate 12 is too weak, and the protective film 16 of the outer edge 12c of the supporting substrate 12 is rolled up during transportation, causing foreign matter A large amount is attached to the outer peripheral portion of the polyimide resin layer 14. Due to the foreign matter, the possibility of damage or the like in the polyimide resin layer 14 is increased. If the second adhesion force F 2 exceeds F 1 (N/10 mm)+0.3 N/10 mm, the adhesion force between the protective film 16 and the support base 12 is too strong. When the protective film 16 is peeled off, use the polyimide resin There is a difference in the peeling speed between the layer 14 part and the supporting base 12 part, and undesirable force is applied to the supporting base 12 when the protective film 16 is peeled off, resulting in the destruction of the supporting base 12. In the laminated substrate 10, since the second adhesion force F 2 of the supporting base 12 and the protective film 16 is within the above-mentioned range, the protective film 16 can be peeled off smoothly, and the supporting base 12 is not damaged. Among them, in order to further suppress the generation of foreign matter on the surface 14a of the polyimide resin layer 14 and the breakage of the support base 12, the second adhesion force F 2 is preferably 0.06 to 0.18 N/10 mm, more preferably 0.07 to 0.17 N/10 mm.

另，積層基板10中，較佳為支持基材12與聚醯亞胺樹脂層14之密著力大於上述第1密著力F1 及第2密著力F2 之任一者。作為提高支持基材12與聚醯亞胺樹脂層14之密著力之方法，如後所述，係改質支持基材12之表面之方法(例如以矽烷偶合劑進行改質之方法)。即，可例舉於支持基材12與聚醯亞胺樹脂層14間，設置矽烷偶合劑層(設置使用矽烷偶合劑形成之層)之方法、或於支持基材12與聚醯亞胺樹脂層14間，設置提高兩者之密著性之層(例如，後述之矽酮樹脂層)之方法。 另，於支持基材12與聚醯亞胺樹脂層14間設置有如矽烷偶合劑層及矽酮樹脂層般之層之情形時，較佳為支持基材12與矽烷偶合劑層或矽酮樹脂層之密著力、及聚醯亞胺樹脂層14與矽烷偶合劑層或矽酮樹脂層之密著力大於上述第1密著力F1 及第2密著力F2 之任一者。In addition, in the laminated substrate 10, it is preferable that the adhesion force between the support base 12 and the polyimide resin layer 14 is greater than any one of the first adhesion force F 1 and the second adhesion force F 2 described above. As a method of improving the adhesion between the support substrate 12 and the polyimide resin layer 14, as described later, a method of modifying the surface of the support substrate 12 (for example, a method of modifying with a silane coupling agent). That is, a method of disposing a silane coupling agent layer (a layer formed using a silane coupling agent) between the supporting base 12 and the polyimide resin layer 14 can be exemplified, or between the supporting base 12 and the polyimide resin Between the layers 14, a method of providing a layer (for example, a silicone resin layer described later) that improves the adhesion between the two. In addition, when a layer such as a silane coupling agent layer and a silicone resin layer is provided between the supporting substrate 12 and the polyimide resin layer 14, it is preferable to support the substrate 12 and the silane coupling agent layer or the silicone resin. The adhesive force of the layer and the adhesive force of the polyimide resin layer 14 and the silane coupling agent layer or the silicone resin layer are greater than any one of the first adhesive force F 1 and the second adhesive force F 2.

[積層基板之第1例之製造方法] 作為製造第1例之積層基板10之方法，較佳為於支持基材12之表面12a上，積層聚醯亞胺樹脂層14之方法。其中，較佳為於支持基材12之表面12a上積層聚醯亞胺樹脂層14之前，於支持基材12之表面12a上塗佈眾所周知之矽烷偶合劑，其後，於塗佈有矽烷偶合劑之支持基材12之表面12a上，積層聚醯亞胺樹脂層14。該情形時，於支持基材12與聚醯亞胺樹脂層14間，設置有矽烷偶合劑層。於支持基材12之表面12a上形成有聚醯亞胺樹脂層14之狀態下，將密著層19朝向支持基材12之表面12a地配置保護膜16，將覆蓋聚醯亞胺樹脂層14之保護膜16貼附於支持基材12。藉此，可製造積層基板10。[Manufacturing method of the first example of multilayer substrate] As a method of manufacturing the laminated substrate 10 of the first example, a method of laminating the polyimide resin layer 14 on the surface 12a of the support base 12 is preferable. Among them, it is preferable to coat a well-known silane coupling agent on the surface 12a of the support substrate 12 before laminating the polyimide resin layer 14 on the surface 12a of the support substrate 12, and then apply a silane coupling agent to the surface 12a of the support substrate 12. A polyimide resin layer 14 is laminated on the surface 12a of the supporting substrate 12 of the mixture. In this case, a silane coupling agent layer is provided between the support base 12 and the polyimide resin layer 14. In the state where the polyimide resin layer 14 is formed on the surface 12a of the support substrate 12, the protective film 16 is arranged so that the adhesion layer 19 faces the surface 12a of the support substrate 12 to cover the polyimide resin layer 14 The protective film 16 is attached to the supporting substrate 12. Thereby, the multilayer substrate 10 can be manufactured.

[積層基板之第2例] 圖4係模式性顯示本發明之實施形態之積層基板之第2例之俯視圖。另，圖4所示之第2例之積層基板10中，對與圖1及圖2所示之第1例之積層基板10同一之構成物標註同一符號，省略其詳細之說明。 第2例之積層基板10與圖1及圖2所示之積層基板10相比，除了保護膜16之大小大於支持基材12以外，皆與圖1及圖2所示之積層基板10相同。 如第2例之積層基板10，藉由使保護膜16之大小大於支持基材12，可於剝離保護膜16時，容易固持保護膜16之一端部。[The second example of multilayer substrate] Fig. 4 is a plan view schematically showing the second example of the multilayer substrate of the embodiment of the present invention. In addition, in the laminated substrate 10 of the second example shown in FIG. 4, the same components as those of the laminated substrate 10 of the first example shown in FIGS. 1 and 2 are denoted by the same reference numerals, and detailed descriptions thereof are omitted. Compared with the laminated substrate 10 shown in FIGS. 1 and 2, the laminated substrate 10 of the second example is the same as the laminated substrate 10 shown in FIGS. 1 and 2 except that the size of the protective film 16 is larger than the supporting base 12. Like the laminated substrate 10 of the second example, by making the size of the protective film 16 larger than the supporting base 12, it is easy to hold one end of the protective film 16 when the protective film 16 is peeled off.

[積層基板之第2例之製造方法] 第2例之積層基板10除了對保護膜16使用大於支持基材12者，將保護膜16覆蓋聚醯亞胺樹脂層14地貼附於支持基材12之點以外，皆可以與第1例之積層基板10同樣之方法製造。[Manufacturing method of the second example of multilayer substrate] The laminated substrate 10 of the second example can be used in the same way as the first example except that the protective film 16 is larger than the supporting base 12, and the protective film 16 is covered with the polyimide resin layer 14 and attached to the supporting base 12. The laminated substrate 10 is manufactured in the same way.

[積層基板之第3例] 圖5係模式性顯示本發明之實施形態之積層基板之第3例之剖視圖。另，圖5所示之第3例之積層基板10中，對與圖1及圖2所示之第1例之積層基板10同一之構成物標註同一符號，省略其詳細之說明。 第3例之積層基板10與圖1及圖2所示之積層基板10相比，除了於支持基材12與聚醯亞胺樹脂層14間具有矽酮樹脂層13以外，皆與圖1及圖2所示之積層基板10相同。[The third example of multilayer substrate] Fig. 5 is a cross-sectional view schematically showing a third example of the multilayer substrate of the embodiment of the present invention. In addition, in the multilayer substrate 10 of the third example shown in FIG. 5, the same components as those of the multilayer substrate 10 of the first example shown in FIGS. 1 and 2 are denoted by the same reference numerals, and detailed descriptions thereof are omitted. The laminated substrate 10 of the third example is compared with the laminated substrate 10 shown in FIGS. 1 and 2, except for the silicone resin layer 13 between the support base 12 and the polyimide resin layer 14. The laminated substrate 10 shown in FIG. 2 is the same.

第3例之積層基板10中，依序積層有支持基材12、矽酮樹脂層13、及聚醯亞胺樹脂層14。於支持基材12之表面12a設置有矽酮樹脂層13，於矽酮樹脂層13之表面13a設置有聚醯亞胺樹脂層14。雖矽酮樹脂層13與聚醯亞胺樹脂層14為相同之大小，但與支持基材12之表面12a相比更小。 第3例之積層基板10中，支持基材12及矽酮樹脂層13作為補強聚醯亞胺樹脂層14之補強板發揮功能。In the laminated substrate 10 of the third example, a supporting base 12, a silicone resin layer 13, and a polyimide resin layer 14 are laminated in this order. A silicone resin layer 13 is provided on the surface 12 a of the support base 12, and a polyimide resin layer 14 is provided on the surface 13 a of the silicone resin layer 13. Although the silicone resin layer 13 and the polyimide resin layer 14 have the same size, they are smaller than the surface 12a of the support substrate 12. In the laminated substrate 10 of the third example, the supporting base 12 and the silicone resin layer 13 function as a reinforcing plate for reinforcing the polyimide resin layer 14.

對積層基板10實施加熱處理之情形時，較佳為使支持基材12與矽酮樹脂層13間之密著力大於矽酮樹脂層13與聚醯亞胺樹脂層14間之密著力。此可藉由以加熱處理，使支持基材12之羥基與矽酮樹脂層13之羥基鍵结等而產生。 其結果，若對剝離支持基材12與聚醯亞胺樹脂層14之方向施加力，則於矽酮樹脂層13與聚醯亞胺樹脂層14間發生剝離。藉此，可將聚醯亞胺樹脂層14分離。 另，第3例之積層基板10中，關於保護膜16之大小無限制。可與圖1所示之積層基板10同樣，使保護膜16與支持基材12為相同之大小，亦可與圖4所示之積層基板10同樣，使保護膜16之大小大於支持基材12。When heat treatment is performed on the laminated substrate 10, it is preferable that the adhesion force between the support base 12 and the silicone resin layer 13 be greater than the adhesion force between the silicone resin layer 13 and the polyimide resin layer 14. This can be produced by bonding the hydroxyl groups of the supporting substrate 12 with the hydroxyl groups of the silicone resin layer 13 by heat treatment. As a result, if a force is applied in the direction in which the support base 12 and the polyimide resin layer 14 are peeled off, peeling occurs between the silicone resin layer 13 and the polyimide resin layer 14. Thereby, the polyimide resin layer 14 can be separated. In addition, in the multilayer substrate 10 of the third example, the size of the protective film 16 is not limited. The protective film 16 and the supporting base 12 may be the same size as the laminated substrate 10 shown in FIG. 1, or the protective film 16 may be larger than the supporting base 12 in the same size as the laminated substrate 10 shown in FIG. .

[積層基板之第3例之製造方法] 製造第3例之積層基板10之方法較佳為於聚醯亞胺樹脂層14之背面(與表面14a相反側之面)形成矽酮樹脂層13之方法。具體而言，較佳為如下方法：將包含硬化性矽酮之硬化性組合物塗佈於聚醯亞胺樹脂層14之背面，對所得之塗膜實施硬化處理，獲得矽酮樹脂層13後，於矽酮樹脂層13之背面(與表面13a相反側之面)積層支持基材12，製造積層基板10。 更詳細而言，製造第3例之積層基板10之方法至少具有如下步驟：將硬化性矽酮層形成於聚醯亞胺樹脂層14之背面(與表面14a相反側之面)，於聚醯亞胺樹脂層14之背面形成矽酮樹脂層13之步驟(樹脂層形成步驟)；於矽酮樹脂層13之背面(與表面13a相反側之面)積層支持基材12之步驟(積層步驟)；及貼附保護膜16之步驟(貼合步驟)。以下，針對上述各步驟詳細敘述。[Manufacturing method of the third example of multilayer substrate] The method of manufacturing the multilayer substrate 10 of the third example is preferably a method of forming the silicone resin layer 13 on the back surface of the polyimide resin layer 14 (the surface opposite to the surface 14a). Specifically, the following method is preferred: a curable composition containing curable silicone is applied to the back surface of the polyimide resin layer 14, and the resulting coating film is cured to obtain the silicone resin layer 13. , The support base 12 is laminated on the back surface of the silicone resin layer 13 (the side opposite to the surface 13a) to produce a laminated substrate 10. In more detail, the method of manufacturing the multilayer substrate 10 of the third example has at least the following steps: a curable silicone layer is formed on the back surface of the polyimide resin layer 14 (the surface opposite to the surface 14a), and The step of forming the silicone resin layer 13 on the back of the imine resin layer 14 (resin layer forming step); the step of laminating the support base 12 on the back of the silicone resin layer 13 (the side opposite to the surface 13a) (the laminating step) ; And the step of attaching the protective film 16 (the step of attaching). Hereinafter, the above-mentioned steps will be described in detail.

(樹脂層形成步驟) 樹脂層形成步驟係將硬化性矽酮層形成於聚醯亞胺樹脂層14之背面，而於聚醯亞胺樹脂層14之背面形成矽酮樹脂層13之步驟。藉由本步驟，獲得依序具備聚醯亞胺樹脂層14與矽酮樹脂層13之附矽酮樹脂層之基板。 附矽酮樹脂層之基板可以於捲繞成捲狀之聚醯亞胺樹脂層14之背面形成矽酮樹脂層13後，再次捲繞成捲狀之所謂之捲對捲方式製造，從而生產效率優良。 本步驟中，為了於聚醯亞胺樹脂層14之背面形成硬化性矽酮層，而將上述之硬化性組合物塗佈於聚醯亞胺樹脂層14之背面。接著，較佳為藉由對硬化性矽酮層實施硬化處理而形成硬化層。 作為於聚醯亞胺樹脂層14之背面塗佈硬化性組合物之方法之具體例，可例舉噴塗法、模塗法、旋塗法、浸漬塗佈法、輥塗法、棒塗法、網版印刷法及凹版印刷塗佈法。 接著，使塗佈於聚醯亞胺樹脂層14之背面之硬化性矽酮硬化，而形成矽酮樹脂層13。(Resin layer formation step) The resin layer forming step is a step of forming a curable silicone layer on the back surface of the polyimide resin layer 14 and forming a silicone resin layer 13 on the back surface of the polyimide resin layer 14. Through this step, a substrate with a silicone resin layer including a polyimide resin layer 14 and a silicone resin layer 13 in this order is obtained. The substrate with a silicone resin layer can be manufactured by the so-called roll-to-roll method in which the silicone resin layer 13 is formed on the back side of the polyimide resin layer 14 wound into a roll shape, and then wound into a roll shape again to achieve production efficiency. excellent. In this step, in order to form a curable silicone layer on the back surface of the polyimide resin layer 14, the curable composition described above is applied to the back surface of the polyimide resin layer 14. Next, it is preferable to form a hardened layer by subjecting the hardenable silicone layer to hardening treatment. As a specific example of the method of coating the curable composition on the back surface of the polyimide resin layer 14, spray coating method, die coating method, spin coating method, dip coating method, roll coating method, bar coating method, Screen printing method and gravure printing coating method. Next, the curable silicone coated on the back surface of the polyimide resin layer 14 is cured to form the silicone resin layer 13.

用以形成矽酮樹脂層13之硬化方法未特別限定，根據使用之硬化性矽酮之種類適當實施最佳之處理。例如，使用縮合反應型矽酮適當及附加反應型矽酮之情形時，作為硬化處理，較佳為熱硬化處理。 熱硬化處理之條件於聚醯亞胺樹脂層14之耐熱性之範圍內實施，例如，熱硬化之溫度條件較佳為50～400°C，更佳為100～300°C。加熱時間較佳為10～300分鐘，更佳為20～120分鐘。 關於矽酮樹脂層13於下文進行說明。The curing method for forming the silicone resin layer 13 is not particularly limited, and the best treatment is appropriately performed according to the type of curable silicone used. For example, when a condensation reaction type silicone is used appropriately and a reaction type silicone is added, the hardening treatment is preferably a thermal hardening treatment. The conditions of the thermal curing treatment are implemented within the range of the heat resistance of the polyimide resin layer 14. For example, the temperature conditions of the thermal curing are preferably 50-400°C, more preferably 100-300°C. The heating time is preferably 10 to 300 minutes, more preferably 20 to 120 minutes. The silicone resin layer 13 will be described below.

(積層步驟) 積層步驟為於矽酮樹脂層13之表面積層支持基材12之步驟。作為將支持基材12積層於矽酮樹脂層13之背面上之方法之具體例，可例舉於常壓環境下，於矽酮樹脂層13之背面上重疊支持基材12之方法。亦可視需要於矽酮樹脂層13之背面上重疊支持基材12後，使用輥或按壓件將支持基材12壓接於矽酮樹脂層13。藉由輥或按壓件之壓接，相對容易地去除混入至矽酮樹脂層13與支持基材12間之氣泡，因而較佳。 若利用真空層壓法或真空按壓法進行壓接，則可抑制氣泡之混入，且實現良好密接，因而較佳。藉由於真空下進行壓接，還有即使於微小氣泡殘留之情形時，氣泡亦不易因加熱處理而成長之優點。 積層支持基材12時，較佳為充分清洗與矽酮樹脂層13接觸之支持基材12之表面，而於清潔度較高之環境下積層。(Layering Steps) The laminating step is a step of supporting the base material 12 on the surface area of the silicone resin layer 13. As a specific example of the method of laminating the supporting substrate 12 on the back surface of the silicone resin layer 13, a method of overlaying the supporting substrate 12 on the back surface of the silicone resin layer 13 in a normal pressure environment can be exemplified. Optionally, after overlaying the supporting substrate 12 on the back surface of the silicone resin layer 13 as needed, the supporting substrate 12 can be crimped to the silicone resin layer 13 by using a roller or a pressing member. It is better to remove air bubbles mixed between the silicone resin layer 13 and the supporting substrate 12 by pressing with a roller or a pressing member. If pressure bonding is performed by a vacuum lamination method or a vacuum pressing method, mixing of bubbles can be suppressed and good adhesion can be achieved, which is preferable. Due to the pressure bonding under vacuum, there is an advantage that even when tiny bubbles remain, the bubbles are not easy to grow due to heat treatment. When laminating the supporting substrate 12, it is preferable to sufficiently clean the surface of the supporting substrate 12 in contact with the silicone resin layer 13, and to laminate in a relatively clean environment.

(貼合步驟) 貼合步驟係將密著層19朝向支持基材12之表面12a地配置保護膜16，覆蓋聚醯亞胺樹脂層14而將保護膜16貼附於支持基材12。藉此，獲得積層基板10。(Fitting step) In the bonding step, the protective film 16 is arranged so that the adhesion layer 19 faces the surface 12 a of the support base 12, covers the polyimide resin layer 14, and the protective film 16 is attached to the support base 12. In this way, a build-up substrate 10 is obtained.

＜捆包體＞ 圖6係模式性顯示本發明之實施形態之捆包體之一例之側視圖。圖6所示之捆包體20中，對與圖1及圖2所示之第1例之積層基板10同一之構成物標註同一符號，省略其詳細之說明。 捆包體20具有上述圖1所示之複數片積層基板10、與積層裝載複數片積層基板10之托板22。 積層基板10為1200 mm×1000 mm(G5尺寸)以上時，難以於積層基板彼此完全分開之狀態下，將之捆包於盒體內，而較佳如後所述，將複數片積層基板10以相互施加荷重之狀態裝載於托板22，並將積層基板10捆包。 積層基板10為四角形，作為積層基板10之大小，較佳為短邊850 mm以上，長邊1100 mm以上，更佳為短邊1200 mm以上，長邊1300 mm以上，進而更佳為短邊1400 mm以上，長邊1700 mm以上。作為積層基板10之大小之上限值，較佳為3000 mm×3000 mm。＜Packing body＞ Fig. 6 is a side view schematically showing an example of the packing body of the embodiment of the present invention. In the package 20 shown in Fig. 6, the same components as those of the laminated substrate 10 of the first example shown in Figs. 1 and 2 are denoted by the same reference numerals, and detailed descriptions thereof are omitted. The package body 20 has a plurality of laminated substrates 10 shown in FIG. 1 and a pallet 22 on which the plurality of laminated substrates 10 are stacked. When the build-up substrate 10 is 1200 mm×1000 mm (G5 size) or more, it is difficult to pack the build-up substrates in a box in a state where they are completely separated from each other. It is mounted on the pallet 22 in a state where the load is applied to each other, and the laminated substrate 10 is bundled. The laminated substrate 10 has a quadrangular shape. As the size of the laminated substrate 10, the short side is preferably 850 mm or more, the long side is 1100 mm or more, more preferably the short side is 1200 mm or more, the long side is 1300 mm or more, and the short side is 1400 mm or more. More than 1700 mm on the long side. The upper limit of the size of the build-up substrate 10 is preferably 3000 mm×3000 mm.

托板22具有底板24與背板26，於底板24立設有背板26。底板24之表面24a與背板26之表面26a正交。將積層基板10之支持基材12朝向背板26之表面26a地，將支持基材12架於底板24之表面24a與背板26之表面26a，而將例如最靠托板22側之積層基板10以積層基板10傾斜之狀態積層於托板22。積層基板10之支持基材12之背面12b與底板24之表面24a所成之角β之角度為例如45°～85°。 將其他積層基板10之支持基材12接觸重疊於積層基板10之保護膜16上，而將複數片積層基板10接觸積層。 托板22以聚丙烯樹脂等樹脂構成，但未特別限定。 若複數片積層基板10為相互施加荷重之狀態，則可使之相互直接接觸，而裝載於托板22，又，亦可如後所述，於積層基板10間設置襯紙，而將複數片積層基板10裝載於托板22。 又，以將支持基材12之背面12b與相鄰之積層基板10之保護膜16之表面分開為目的，將襯紙放入其等中間。藉由放入襯紙，減少支持基材12之背面12b與相鄰之積層基板10之保護膜16之表面的密著，從而於自托板22拿取積層基板10之情形時，可容易地逐片拿取。The supporting plate 22 has a bottom plate 24 and a back plate 26, and a back plate 26 is erected on the bottom plate 24. The surface 24 a of the bottom plate 24 is orthogonal to the surface 26 a of the back plate 26. With the supporting base 12 of the build-up substrate 10 facing the surface 26a of the backing plate 26, the supporting base 12 is placed on the surface 24a of the bottom plate 24 and the surface 26a of the backing plate 26, and for example, the build-up substrate closest to the supporting plate 22 is placed 10 is laminated on the pallet 22 in a state where the laminated substrate 10 is inclined. The angle β formed by the back surface 12b of the supporting base 12 of the laminated substrate 10 and the surface 24a of the bottom plate 24 is, for example, 45° to 85°. The supporting base material 12 of the other build-up substrate 10 is contacted and overlapped on the protective film 16 of the build-up substrate 10, and a plurality of the build-up substrates 10 are contacted and laminated. The pallet 22 is made of resin such as polypropylene resin, but is not particularly limited. If a plurality of laminated substrates 10 are in a state where loads are applied to each other, they can be placed in direct contact with each other and mounted on the pallet 22. Furthermore, as will be described later, a backing paper may be provided between the laminated substrates 10, and the plurality of laminated substrates The build-up substrate 10 is mounted on the pallet 22. In addition, for the purpose of separating the back surface 12b of the support base 12 from the surface of the protective film 16 of the adjacent build-up substrate 10, a backing paper is placed in between. By inserting the backing paper, the adhesion between the back surface 12b of the support base 12 and the surface of the protective film 16 of the adjacent build-up substrate 10 is reduced, so that when the build-up substrate 10 is taken from the pallet 22, it can be easily Take one piece by piece.

另，托板22設為具有底板24與背板26之構成，但只要可積層裝載複數片積層基板10，則其之構成無特別限定。 以將複數片積層基板10以相互施加荷重之狀態裝載於托板22之捆包體20之形態，搬送積層基板10。此時，對複數片積層基板10中，最靠背板26側之積層基板10施加最大之荷重，且藉由搬送時之振動，積層基板10彼此摩擦。如上所述，藉由設置保護膜16，即使對積層基板10施加荷重，即使積層基板10彼此摩擦，亦抑制對聚醯亞胺樹脂層14造成打痕及損傷，乃至異物附著。In addition, the pallet 22 has a structure having a bottom plate 24 and a back plate 26, but the structure is not particularly limited as long as a plurality of laminated substrates 10 can be stacked and mounted. The multilayer substrate 10 is conveyed in a form in which a plurality of laminated substrates 10 are mounted on the package 20 of the pallet 22 in a state where a load is applied to each other. At this time, the largest load is applied to the multilayer substrate 10 on the side closest to the back plate 26 among the plurality of multilayer substrates 10, and the multilayer substrates 10 rub against each other due to vibration during transportation. As described above, by providing the protective film 16, even if a load is applied to the build-up substrate 10, even if the build-up substrates 10 rub against each other, scratches and damage to the polyimide resin layer 14 and even foreign matter adhesion are suppressed.

積層基板10中，由於支持基材12與保護膜16之第2密著力F2在上述範圍內，故於一般環境中，即使進行捆包體20之輸送，亦不會產生保護膜16與支持基材12之剝離，異物不會大量附著於聚醯亞胺樹脂層14之外周部分，缺陷不會增加。 裝載於托板22之積層基板10並非限定於圖1所示之第1例之積層基板10者，亦可為上述第2例之積層基板10及上述第3例之積層基板10。 又，積層基板10可利用例如日本專利第4251290號公報所記載之玻璃板捆包箱(參照圖1～圖17)捆包。In the laminated substrate 10, since the second adhesion force F2 between the supporting base material 12 and the protective film 16 is within the above range, in a general environment, even if the package 20 is transported, the protective film 16 and the supporting base will not be produced. When the material 12 is peeled off, a large amount of foreign matter will not adhere to the outer peripheral portion of the polyimide resin layer 14, and defects will not increase. The build-up substrate 10 mounted on the pallet 22 is not limited to the build-up substrate 10 of the first example shown in FIG. 1, and may be the build-up substrate 10 of the second example and the build-up substrate 10 of the third example. In addition, the laminated substrate 10 can be packaged using, for example, a glass plate packing box (see FIGS. 1 to 17) described in Japanese Patent No. 4251290.

玻璃板捆包箱具體而言以排列載置積層基板10之台座、載置該台座之底板、豎立配設於底板上之前板、後板及兩側板、及蓋住上部之頂板構成。 玻璃板捆包箱於底板之上部前緣及兩側緣，具備用以嵌入前板及兩側板之安裝構件。安裝構件於底面板設置有對向之1對側板，於對向之側板間，嵌入前板及兩側板。安裝構件除上述構成以外，亦可設為於底板設置上方開口之槽，於該槽嵌入前板及兩側板之構造。 又，為了防止載置積層基板時之損傷，亦可於底承板及背承板分別貼附緩衝材。 又，亦可於將複數片積層基板載置於台座後，以樹脂製等之保護板覆蓋包含複數片積層基板之收納體之前側，於兩角部配設三角材，並將該等用帶捆紮。該帶將可調節長度之皮帶構件之端部所配備之固定金屬件與肘夾扣合等，而確實地捆紮收納體。如此，藉由使用帶捆紮收納體，可以簡單之機構牢固地固定全體。又，若將保護板設為具有緩衝性之構件，則以帶捆紮積層基板後，可進而強固地捆紮肘夾。Specifically, the glass plate packing box is composed of a pedestal on which the laminated substrate 10 is placed, a bottom plate on which the pedestal is placed, a front plate, a rear plate, and both side plates vertically arranged on the bottom plate, and a top plate covering the upper part. The glass plate packing box is equipped with installation members for embedding the front plate and the two side plates on the front edge and both side edges of the upper part of the bottom plate. The mounting member is provided with a pair of opposite side panels on the bottom panel, and the front panel and both side panels are embedded between the opposite side panels. In addition to the above-mentioned structure, the mounting member can also be provided with an upper opening groove on the bottom plate, and a structure in which the front plate and both side plates are inserted into the groove. In addition, in order to prevent damage when placing the laminated substrate, a cushioning material may be attached to the bottom support plate and the back support plate, respectively. In addition, after placing a plurality of laminated substrates on the pedestal, cover the front side of the storage body containing the plurality of laminated substrates with a protective plate made of resin, etc., arrange triangular materials on both corners, and attach the tapes Strapping. The belt buckles the fixed metal parts provided at the end of the belt member with adjustable length with the elbow clip, etc., and securely binds the storage body. In this way, by tying the storage body with a belt, the whole can be firmly fixed with a simple mechanism. In addition, if the protective plate is used as a member having cushioning properties, the elbow clamp can be further firmly tied after the laminated substrate is tied with a tape.

以下，針對構成積層基板10之支持基材12、聚醯亞胺樹脂層14、矽酮樹脂層13及保護膜16詳細敘述。Hereinafter, the supporting base 12, the polyimide resin layer 14, the silicone resin layer 13, and the protective film 16 constituting the laminated substrate 10 will be described in detail.

＜支持基材＞ 玻璃製之支持基材12為支持並補強聚醯亞胺樹脂層14之構件，且作為搬送基板發揮功能。支持基材12以例如玻璃板構成。 作為玻璃之種類，較佳為無鹼硼矽酸玻璃、硼矽酸玻璃、鈉鈣玻璃、高二氧化矽玻璃、以其他氧化矽為主成分之氧化物系玻璃。作為氧化物系玻璃，較佳為利用氧化物換算之氧化矽含量為40～90質量%之玻璃。 作為玻璃，更具體而言，可例舉包含無鹼硼矽酸玻璃之玻璃板(AGC股份有限公司製，商品名「AN100」)。 作為玻璃板之製造方法，可例舉通常將玻璃原料熔融，將熔融玻璃成形為板狀之方法。此種成形方法可為一般者，可例舉例如浮式法、熔融法及流孔下引法。＜Support base material＞ The supporting substrate 12 made of glass is a member that supports and reinforces the polyimide resin layer 14 and functions as a transport substrate. The supporting substrate 12 is constituted by, for example, a glass plate. The type of glass is preferably alkali-free borosilicate glass, borosilicate glass, soda lime glass, high silica glass, and oxide-based glass mainly composed of other silica. As the oxide-based glass, a glass having a silicon oxide content of 40 to 90% by mass in terms of oxide is preferred. As the glass, a glass plate containing alkali-free borosilicate glass (manufactured by AGC Co., Ltd., trade name "AN100") can be mentioned more specifically. As a manufacturing method of a glass plate, the method of generally melting glass raw materials and shaping the molten glass into a plate shape can be mentioned. Such a forming method may be general, and examples thereof include a float method, a melting method, and a flow hole down-drawing method.

支持基材12之厚度可厚於或薄於聚醯亞胺樹脂層14。基於積層基板10之處理性之點，較佳使支持基材12之厚度厚於聚醯亞胺樹脂層14。 由於支持基材12係要求作為補強板及搬送基板之功能者，故較佳為非可撓性。因此，支持基材12之厚度較佳為0.3 mm以上，更佳為0.5 mm以上。另一方面，支持基材12之厚度較佳為1.0 mm以下。The thickness of the supporting substrate 12 may be thicker or thinner than the polyimide resin layer 14. Based on the rationality of the laminated substrate 10, it is preferable to make the thickness of the support base 12 thicker than the polyimide resin layer 14. Since the supporting base 12 is required to function as a reinforcing plate and a substrate for conveying, it is preferably inflexible. Therefore, the thickness of the supporting substrate 12 is preferably 0.3 mm or more, more preferably 0.5 mm or more. On the other hand, the thickness of the support base 12 is preferably 1.0 mm or less.

＜聚醯亞胺樹脂層＞ 聚醯亞胺樹脂層14包含聚醯亞胺樹脂，且使用例如聚醯亞胺薄膜。作為聚醯亞胺薄膜之市售品之具體例，可例舉東洋紡股份有限公司製之「XENOMAX」，宇部興產股份有限公司製之「UPILEX 25S」。 為了形成構成電子裝置之高精細配線等，聚醯亞胺樹脂層14之表面14a平滑。具體而言，聚醯亞胺樹脂層14之表面14a之表面粗糙度Ra較佳為50 nm以下，更佳為30 nm以下，進而更佳為10 nm以下。作為表面粗糙度Ra之下限，可例舉0.01 nm以上。 基於製造步驟之操作性之點，聚醯亞胺樹脂層14之厚度較佳為1 μm以上，更佳為5 μm以上，進而更佳為10 μm以上。基於柔軟性之點，聚醯亞胺樹脂層14之厚度較佳為1 mm以下，更佳為0.2 mm以下。 由於聚醯亞胺樹脂層14之熱膨脹係數與支持基材12之熱膨脹係數之差較小者可抑制加熱後或冷卻後之撓曲，因而較佳。具體而言，聚醯亞胺樹脂層14與支持基材12之熱膨脹係數之差較佳為0～90×10-6 /°C，更佳為0～30×10-6 /°C。<Polyimide resin layer> The polyimide resin layer 14 contains a polyimide resin, and a polyimide film is used, for example. Specific examples of commercially available polyimide films include "XENOMAX" manufactured by Toyobo Co., Ltd. and "UPILEX 25S" manufactured by Ube Kosan Co., Ltd. In order to form high-definition wiring and the like constituting an electronic device, the surface 14a of the polyimide resin layer 14 is smooth. Specifically, the surface roughness Ra of the surface 14a of the polyimide resin layer 14 is preferably 50 nm or less, more preferably 30 nm or less, and even more preferably 10 nm or less. As the lower limit of the surface roughness Ra, 0.01 nm or more can be mentioned. Based on the operability of the manufacturing process, the thickness of the polyimide resin layer 14 is preferably 1 μm or more, more preferably 5 μm or more, and even more preferably 10 μm or more. Based on flexibility, the thickness of the polyimide resin layer 14 is preferably 1 mm or less, more preferably 0.2 mm or less. Since the difference between the coefficient of thermal expansion of the polyimide resin layer 14 and the coefficient of thermal expansion of the support base 12 is smaller, the deflection after heating or cooling can be suppressed, which is preferable. Specifically, the difference in thermal expansion coefficient between the polyimide resin layer 14 and the support base 12 is preferably 0 to 90×10 -6 /°C, more preferably 0 to 30×10 -6 /°C.

聚醯亞胺樹脂層14之面積(表面14a之面積)雖未特別限制，但為了配置保護膜16，較佳為小於支持基材12之面積。另一方面，基於電子裝置之生產性之點，聚醯亞胺樹脂層14之面積較佳為300 cm2 以上。 聚醯亞胺樹脂層14之形狀未特別限制，可為矩形狀亦可為圓形狀。又可於聚醯亞胺樹脂層14，形成定向平面(形成於基板外周之平坦部分)、及凹口(形成於基板之外周緣之至少1個V型缺口)。Although the area of the polyimide resin layer 14 (the area of the surface 14a) is not particularly limited, in order to arrange the protective film 16, it is preferably smaller than the area of the support base 12. On the other hand, based on the productivity of the electronic device, the area of the polyimide resin layer 14 is preferably 300 cm 2 or more. The shape of the polyimide resin layer 14 is not particularly limited, and may be rectangular or circular. In addition, the polyimide resin layer 14 can be formed with an orientation plane (a flat part formed on the outer periphery of the substrate) and a notch (at least one V-shaped notch formed on the outer periphery of the substrate).

＜保護膜＞ 保護膜16如圖3所示，較佳為具有基材18與密著層19之積層構造。 為了減少自外部受到之力之影響，保護膜16之厚度較佳為20μm以上，更佳為30 μm以上，進而更佳為50 μm以上。作為保護膜16之厚度之上限值，較佳為500 μm以下，更佳為300 μm以下，進而更佳為100 μm以下。 於具有基材18與密著層19之積層構造之情形時，保護膜16之厚度為基材18與密著層19之合計厚度。作為保護膜16之厚度之上限，若過厚，則有剝離保護膜時需過大之力之情形，故較佳為500 μm以下。 保護膜16之厚度以接觸式膜厚測定裝置，測定5點以上之任意位置之保護膜16之厚度，並將該等進行算數平均者。 又，保護膜16之基材18較佳以聚酯樹脂(例如，聚對苯二甲酸乙二酯(PET))、聚烯烴樹脂(例如，聚乙烯(PE)及聚丙烯等)、聚胺酯樹脂等樹脂構成。其中，作為構成保護膜16之基材18之樹脂，較佳為聚烯烴，更佳為聚乙烯或聚丙烯。 若密著層19滿足上述第1密著力F1 及上述第2密著力F2 ，則並無特別限定。作為密著層19，亦可使用眾所周知之黏著層。作為構成黏著層之黏著劑之具體例，可例舉(甲基)丙烯酸系黏著劑、矽酮系黏著劑、胺基甲酸酯系黏著劑。 又，密著層19亦可以樹脂構成，作為樹脂之具體例，可例舉乙酸乙烯酯樹脂、乙烯-乙酸乙烯酯共聚物樹脂、氯乙烯-乙酸乙烯酯共聚物樹脂、(甲基)丙烯酸樹脂、縮丁醛樹脂、聚胺酯樹脂、聚苯乙烯彈性體等。 另，(甲基)丙烯酸係包含丙烯酸與甲基丙烯酸之概念。<Protective Film> As shown in FIG. 3, the protective film 16 preferably has a laminated structure of the base material 18 and the adhesion layer 19. In order to reduce the influence of the force received from the outside, the thickness of the protective film 16 is preferably 20 μm or more, more preferably 30 μm or more, and even more preferably 50 μm or more. The upper limit of the thickness of the protective film 16 is preferably 500 μm or less, more preferably 300 μm or less, and still more preferably 100 μm or less. In the case of a laminated structure of the base material 18 and the adhesion layer 19, the thickness of the protective film 16 is the total thickness of the base material 18 and the adhesion layer 19. As the upper limit of the thickness of the protective film 16, if it is too thick, excessive force may be required to peel the protective film, so it is preferably 500 μm or less. The thickness of the protective film 16 is measured by a contact-type film thickness measuring device, and the thickness of the protective film 16 at any position above 5 points is measured, and these are calculated and averaged. In addition, the base material 18 of the protective film 16 is preferably made of polyester resin (for example, polyethylene terephthalate (PET)), polyolefin resin (for example, polyethylene (PE), polypropylene, etc.), or polyurethane resin. And other resin composition. Among them, the resin constituting the substrate 18 of the protective film 16 is preferably polyolefin, and more preferably polyethylene or polypropylene. If the adhesion layer 19 satisfies the first adhesion force F 1 and the second adhesion force F 2 , it is not particularly limited. As the adhesion layer 19, a well-known adhesion layer can also be used. Specific examples of the adhesive constituting the adhesive layer include (meth)acrylic adhesives, silicone adhesives, and urethane adhesives. In addition, the adhesion layer 19 may also be made of resin. Specific examples of the resin include vinyl acetate resin, ethylene-vinyl acetate copolymer resin, vinyl chloride-vinyl acetate copolymer resin, and (meth)acrylic resin. , Butyral resin, polyurethane resin, polystyrene elastomer, etc. In addition, (meth)acrylic acid includes the concepts of acrylic acid and methacrylic acid.

另，根據保護膜16之種類，聚醯亞胺樹脂層14之表面14a中產生埋設物之難易度改變。以下，針對其機制詳細敘述。 此處，圖7～圖9係模式性說明本發明之實施形態之積層基板之埋設物的產生之剖視圖。又，圖10係顯示本發明之實施形態之積層基板之埋設物之一例之SEM像。另，圖7～圖10中，對與圖1及圖2所示之積層基板10同一之構成物標註同一符號，省略其詳細之說明。 如圖7所示，於聚醯亞胺樹脂層14之表面14a與保護膜16間有異物D之情形時，若保護膜16較硬，則如圖8所示，保護膜16不易變形，導致異物D被埋於聚醯亞胺樹脂層14中。其結果，於聚醯亞胺樹脂層14中產生埋設物。具體而言，如圖10所示之SEM像，異物D被埋於聚醯亞胺樹脂層14，該異物D成為埋設物。 另一方面，若保護膜16較軟，則如圖9所示，保護膜16變形，異物D附著於保護膜16側，異物D不附著於聚醯亞胺樹脂層14，且異物D亦未被埋於聚醯亞胺樹脂層14中。藉此，即使於聚醯亞胺樹脂層14之表面14a與保護膜16間存在異物D而積層，亦抑制聚醯亞胺樹脂層14產生缺陷。因此，保護膜16之基材18較佳為柔軟者。 另，保護膜16之基材18之柔軟度係根據異物D之大小或異物D之硬度等之相對關係決定者。 另，關於上述保護膜16之柔軟度，如後所述，評估實施例之例4～6。In addition, depending on the type of the protective film 16, the difficulty of embedding on the surface 14 a of the polyimide resin layer 14 changes. The mechanism will be described in detail below. Here, FIGS. 7 to 9 are cross-sectional views schematically illustrating the generation of embedded objects in the multilayer substrate according to the embodiment of the present invention. In addition, FIG. 10 is an SEM image showing an example of the embedded object of the multilayer substrate according to the embodiment of the present invention. In addition, in FIGS. 7 to 10, the same components as those of the laminated substrate 10 shown in FIGS. 1 and 2 are denoted by the same reference numerals, and detailed descriptions thereof are omitted. As shown in FIG. 7, when there is a foreign substance D between the surface 14a of the polyimide resin layer 14 and the protective film 16, if the protective film 16 is hard, as shown in FIG. 8, the protective film 16 is not easily deformed, resulting in The foreign matter D is buried in the polyimide resin layer 14. As a result, embedded objects are generated in the polyimide resin layer 14. Specifically, in the SEM image shown in FIG. 10, the foreign matter D is buried in the polyimide resin layer 14, and the foreign matter D becomes the buried object. On the other hand, if the protective film 16 is soft, as shown in FIG. 9, the protective film 16 is deformed, the foreign matter D adheres to the side of the protective film 16, the foreign matter D does not adhere to the polyimide resin layer 14, and the foreign matter D is not It is buried in the polyimide resin layer 14. Thereby, even if a foreign substance D exists between the surface 14a of the polyimide resin layer 14 and the protective film 16 and is laminated, the polyimide resin layer 14 is prevented from being defective. Therefore, the base material 18 of the protective film 16 is preferably soft. In addition, the softness of the base material 18 of the protective film 16 is determined according to the relative relationship between the size of the foreign matter D or the hardness of the foreign matter D. In addition, regarding the softness of the protective film 16, as described later, Examples 4 to 6 of the examples were evaluated.

＜矽酮樹脂層＞ 矽酮樹脂層13為主要包含矽酮樹脂者。矽酮樹脂之構造未特別限制。矽酮樹脂通常將可藉由硬化處理成為矽酮樹脂之硬化性矽酮硬化(交聯硬化)而獲得。 作為硬化性矽酮之具體例，根據其之硬化機製，可例舉縮合反應型矽酮、附加反應型矽酮、紫外線硬化型矽酮及電子束硬化型矽酮。硬化性矽酮之重量平均分子量較佳為5,000～60,000，更佳為5,000～30,000。＜Silicone resin layer＞ The silicone resin layer 13 mainly contains silicone resin. The structure of the silicone resin is not particularly limited. The silicone resin is usually obtained by curing (crosslinking and curing) a curable silicone that is cured into a silicone resin. As specific examples of curable silicone, according to its curing mechanism, condensation reaction type silicone, additive reaction type silicone, ultraviolet curing type silicone, and electron beam curing type silicone can be exemplified. The weight average molecular weight of the curable silicone is preferably 5,000 to 60,000, more preferably 5,000 to 30,000.

作為矽酮樹脂層13之製造方法，較佳為如下方法：於聚醯亞胺樹脂層14之背面(與表面14a相反側之面)塗佈包含成為上述矽酮樹脂之硬化性矽酮之硬化性組合物，視需要去除溶媒，形成塗膜，使塗膜中之硬化性矽酮硬化，而設為矽酮樹脂層13。 硬化性組合物除了硬化性矽酮外，亦可包含溶媒、鉑催化劑(使用附加反應型矽酮作為硬化性矽酮之情形)、調平劑及金屬化合物等。作為金屬化合物所含之金屬元素之具體例，可例舉3d過渡金屬、4d過渡金屬、鑭系金屬、鉍、鋁及錫。適當調整金屬化合物之含量。As a method of manufacturing the silicone resin layer 13, the following method is preferred: the back surface of the polyimide resin layer 14 (the surface opposite to the surface 14a) is coated with curable silicone containing the aforementioned silicone resin. For the sexual composition, the solvent is removed as necessary to form a coating film to harden the curable silicone in the coating film, and set it as the silicone resin layer 13. In addition to the curable silicone, the curable composition may also contain a solvent, a platinum catalyst (in the case of using an additional reactive silicone as the curable silicone), a leveling agent, a metal compound, and the like. Specific examples of metal elements contained in the metal compound include 3d transition metals, 4d transition metals, lanthanide metals, bismuth, aluminum, and tin. Adjust the content of metal compounds appropriately.

矽酮樹脂層13之厚度較佳為100 μm以下，更佳為50 μm以下，進而更佳為30 μm以下。另一方面，矽酮樹脂層13之厚度較佳為超1 μm，更佳為4 μm以上。上述厚度係以接觸式膜厚測定裝置測定5點以上之任意位置之矽酮樹脂層13之厚度，並將該等進行算數平均者。The thickness of the silicone resin layer 13 is preferably 100 μm or less, more preferably 50 μm or less, and still more preferably 30 μm or less. On the other hand, the thickness of the silicone resin layer 13 is preferably more than 1 μm, more preferably 4 μm or more. The above-mentioned thickness is measured by measuring the thickness of the silicone resin layer 13 at any position above 5 points with a contact-type film thickness measuring device, and performing arithmetic average of these.

＜積層基板之用途＞ 作為積層基板10之用途，可例舉後述顯示裝置、接收感測器面板、太陽能電池、薄膜2次電池及積體電路等。亦有將聚醯亞胺樹脂層以剝離保護膜16之狀態於大氣氛圍下，以例如450°C以上之高溫條件，暴露20分鐘以上之情形。 作為顯示裝置之具體例，可例舉LCD、OLED、電子紙、電漿顯示面板、場發射面板、量子點LED面板、微LED顯示器面板及MEMS(Micro Electro Mechanical Systems：微電子機械系統)快門面板。 作為接收感測器面板之具體例，可例舉電磁波接收感測器面板、X射線受光感測器面板、紫外線受光感測器面板、可見光線受光感測器面板及紅外線受光感測器面板。用於接收感測器面板之情形時，亦可藉由樹脂等之補強片等補強聚醯亞胺樹脂層。＜Use of multilayer substrates＞ As the application of the multilayer substrate 10, a display device, a receiving sensor panel, a solar cell, a thin-film secondary cell, an integrated circuit, etc., which will be described later, can be exemplified. There is also a case where the polyimide resin layer is exposed to the atmosphere in a state where the protective film 16 is peeled off under high temperature conditions of, for example, 450° C. or more for more than 20 minutes. Specific examples of display devices include LCD, OLED, electronic paper, plasma display panels, field emission panels, quantum dot LED panels, micro LED display panels, and MEMS (Micro Electro Mechanical Systems) shutter panels . Specific examples of the receiving sensor panel include an electromagnetic wave receiving sensor panel, an X-ray receiving sensor panel, an ultraviolet receiving sensor panel, a visible light receiving sensor panel, and an infrared receiving sensor panel. When used in the case of receiving a sensor panel, the polyimide resin layer can also be reinforced with a reinforcing sheet such as resin.

如上所述，自本發明之積層基板剝離保護膜後，使用獲得之包含支持基材與聚醯亞胺樹脂層之積層體，製造包含聚醯亞胺樹脂層與電子裝置用構件之電子裝置。 作為電子裝置之製造方法，可例舉如下方法：例如於獲得之包含支持基材與聚醯亞胺樹脂層之積層體中之聚醯亞胺樹脂層上，形成電子裝置用構件，將支持基材自獲得之附電子裝置用構件之積層體剝離，獲得具有聚醯亞胺樹脂層與電子裝置用構件之電子裝置。 另，上述電子裝置用構件為構成電子裝置之至少一部分之構件。 [實施例]As described above, after the protective film is peeled off from the laminated substrate of the present invention, the obtained laminated body including the supporting substrate and the polyimide resin layer is used to manufacture an electronic device including the polyimide resin layer and the electronic device member. As a manufacturing method of an electronic device, the following method can be exemplified: for example, a member for the electronic device is formed on the polyimide resin layer in the obtained laminate comprising a support base material and a polyimide resin layer, and the support base is formed on the polyimide resin layer. The material was peeled from the obtained laminate with the electronic device member to obtain an electronic device having the polyimide resin layer and the electronic device member. In addition, the above-mentioned electronic device member is a member that constitutes at least a part of the electronic device. [Example]

於以下，藉由實施例等更具體地說明本發明，但本發明並非受該等例所限制者。後述之例1～6為實施例，例7～16為比較例。In the following, the present invention will be explained in more detail with examples and the like, but the present invention is not limited by these examples. Examples 1 to 6 described later are examples, and examples 7 to 16 are comparative examples.

＜評估＞ (外周部異物評估) 外周部異物評估中，各例中，於設置保護膜前，使用Orbotech公司製光學式檢查裝置，預先取得聚醯亞胺樹脂層之外周部10 mm寬度之邊緣區域表面存在之缺陷的位置資訊及圖像。且，以對各例中獲得之積層基板之保護膜上，施加16 g/cm2 之荷重之狀態，於溫度40°C、相對濕度80%之氛圍中放置5天。其後，剝離保護膜，再次使用Orbotech公司製光學式檢查裝置，取得聚醯亞胺樹脂層之外周部10 mm寬度之邊緣區域表面存在之缺陷之位置資訊及圖像。 比較設置保護膜前後之圖像，評估邊緣區域有無異物。由於除異物以外，亦可能產生黏著劑殘留或損傷之缺陷，故預先定義顯示異物之圖像，且於比較圖像時，參考顯示異物之圖像，評估有無異物。 圖像比較之結果，若外周部有異物，則設為「有」，若外周部無異物，則設為「無」。<Evaluation> (Evaluation of foreign matter in the outer periphery) In the evaluation of foreign matter in the outer periphery, in each case, before installing the protective film, an optical inspection device manufactured by Orbotech was used to obtain a 10 mm width edge of the outer periphery of the polyimide resin layer in advance Location information and images of defects on the surface of the area. In addition, the protective film of the laminated substrate obtained in each example was placed under an atmosphere of a temperature of 40°C and a relative humidity of 80% for 5 days in a state where a load of 16 g/cm 2 was applied. After that, the protective film was peeled off, and an optical inspection device manufactured by Orbotech was used again to obtain position information and images of defects on the surface of the 10 mm width edge area of the outer periphery of the polyimide resin layer. Compare the images before and after setting the protective film to evaluate whether there are foreign objects in the edge area. In addition to foreign objects, there may also be defects such as adhesive residue or damage. Therefore, the image showing the foreign object is defined in advance, and when comparing the images, refer to the image showing the foreign object to evaluate whether there is a foreign object. As a result of image comparison, if there is a foreign matter on the outer periphery, set it as "Yes", and if there is no foreign matter on the outer periphery, set it as "No".

(黏著劑殘留之評估) 黏著劑殘留之評估中，各例中，於設置保護膜前，使用Orbotech公司製光學式檢查裝置，預先取得聚醯亞胺樹脂層表面存在之缺陷之位置資訊及圖像。然後，以對各例中獲得之積層基板之保護膜上，施加16 g/cm2 之荷重之狀態，於溫度40°C、相對濕度80%之氛圍中放置5天。其後，剝離保護膜，再次使用Orbotech公司製光學式檢查裝置，取得聚醯亞胺樹脂層表面存在之缺陷之位置資訊及圖像。 比較設置保護膜前後之圖像，評估有無黏著劑殘留。由於除黏著劑殘留以外，亦可能附有損傷等，故預先定義顯示黏著劑殘留之圖像，且於比較圖像時，參考顯示黏著劑殘留之圖像，評估有無黏著劑殘留。 圖像比較之結果，若有黏著劑殘留，則設為「有」，若無黏著劑殘留，則設為「無」。(Evaluation of adhesive residue) In the evaluation of adhesive residue, in each case, before the protective film is installed, an optical inspection device made by Orbotech is used to obtain the location information and the map of the defects on the surface of the polyimide resin layer in advance. Like. Then, on the protective film of the laminated substrate obtained in each example, a load of 16 g/cm 2 was applied, and placed in an atmosphere at a temperature of 40°C and a relative humidity of 80% for 5 days. After that, the protective film was peeled off, and an optical inspection device manufactured by Orbotech was used again to obtain position information and images of defects on the surface of the polyimide resin layer. Compare the images before and after setting the protective film to evaluate whether there is any adhesive residue. In addition to the adhesive residue, there may be damage, etc. Therefore, the image showing the adhesive residue is defined in advance, and when comparing the images, refer to the image showing the adhesive residue to evaluate whether there is adhesive residue. As a result of image comparison, if there is adhesive residue, set it to "Yes"; if there is no adhesive residue, set it to "None".

(損傷之評估) 損傷之評估中，各例中，於設置保護膜前，使用Orbotech公司製光學式檢查裝置，預先取得聚醯亞胺樹脂層表面存在之缺陷之位置資訊及圖像。 且，以於各例中獲得之積層基板之保護膜上，堆疊23片厚度為2.8 mm之玻璃板施加荷重之狀態，於溫度40°C、相對濕度80%之氛圍中放置5天。其後，剝離保護膜，再次使用Orbotech公司製光學式檢查裝置，取得聚醯亞胺樹脂層表面之圖像。 比較施加荷重前後之圖像，評估有無損傷。由於除損傷以外，亦可能產生黏著劑殘留等，故預先定義顯示損傷之圖像，且於比較圖像時，參考顯示損傷之圖像，評估有無損傷。 圖像比較之結果，若有損傷，則設為「有」，若無損傷，則設為「無」。(Assessment of damage) In the evaluation of damage, in each case, before installing the protective film, an optical inspection device made by Orbotech was used to obtain the position information and images of the defects on the surface of the polyimide resin layer in advance. In addition, 23 glass plates with a thickness of 2.8 mm were stacked on the protective film of the laminated substrate obtained in each example, and the load was placed in an atmosphere with a temperature of 40°C and a relative humidity of 80% for 5 days. After that, the protective film was peeled off, and an optical inspection device manufactured by Orbotech was used again to obtain an image on the surface of the polyimide resin layer. Compare the images before and after the load is applied to evaluate whether there is damage. In addition to damage, adhesive residue may also occur, so the image showing the damage is defined in advance, and when comparing the images, refer to the image showing the damage to evaluate whether there is damage. As a result of image comparison, if there is damage, set it to "Yes", if there is no damage, set it to "None".

(支持基材破損之評估) 將保護膜自各例中獲得之積層基板剝離時，將支持基材產生破損之情形設為「有」，將未產生破損之情形設為「無」。(Support the evaluation of substrate damage) When the protective film was peeled from the laminated substrate obtained in each example, the case where the support base material was damaged was set to "Yes", and the case where no damage occurred was set to "None".

(耐熱試驗之評估) 如下實施保護膜剝離後之積層基板之耐熱性評估。 於黏著劑殘留評估用之積層基板，使用電漿CVD(Chemical Vapor Deposition：化學氣相沈積)法，成膜厚度為200 nm之氮化矽膜(SiNx)。其後，於氮氣氛圍中，進行500°C、10分鐘加熱。加熱後，聚醯亞胺樹脂層未自支持基材剝離之情形時，將耐熱性評估為「○」，發生剝離之情形時，將耐熱性評估為「×」。(Evaluation of heat resistance test) The heat resistance evaluation of the laminated substrate after the protective film was peeled off was performed as follows. The build-up substrate used for the evaluation of the adhesive residue is a silicon nitride film (SiNx) with a thickness of 200 nm using the plasma CVD (Chemical Vapor Deposition) method. Thereafter, heating was performed at 500°C for 10 minutes in a nitrogen atmosphere. After heating, when the polyimide resin layer did not peel off from the supporting substrate, the heat resistance was evaluated as "○", and when peeling occurred, the heat resistance was evaluated as "×".

(埋設異物之評估) 根據保護膜之種類，如下實施異物是否埋設於聚醯亞胺樹脂層之評估。 首先，於設置保護膜前，為了刻意地將異物載置於聚醯亞胺樹脂層上，將聚醯亞胺樹脂層放置於常壓常溫環境後，以Orbotech公司製光學式檢查裝置，實施缺陷(異物)之檢查。其後，於聚醯亞胺樹脂層上設置保護膜，以堆疊23片厚度為2.8 mm之玻璃板而施加荷重之狀態，於溫度40°C、相對濕度80%之氛圍中放置5天。接著，剝離保護膜，於聚醯亞胺樹脂層之表面，再次使用Orbotech公司製光學式檢查裝置，實施聚醯亞胺樹脂層表面之缺陷(異物)檢查。藉由比較保護膜貼合前後之Orbotech公司製光學式檢查裝置之缺陷分佈，確認貼合前聚醯亞胺樹脂層上存在之異物於剝離保護膜後是否仍殘留，其後就殘留之異物，使用光學顯微鏡及掃描型電子顯微鏡(SEM)，實施異物之表面觀察。藉由比較光學顯微鏡之圖像與掃描型電子顯微鏡之圖像，進行是否為埋設異物之判定。(Evaluation of buried foreign objects) According to the type of protective film, the evaluation of whether foreign matter is embedded in the polyimide resin layer is carried out as follows. First, before setting the protective film, in order to deliberately place the foreign matter on the polyimide resin layer, the polyimide resin layer is placed in a normal pressure and room temperature environment, and then the defects are implemented with an optical inspection device manufactured by Orbotech. (Foreign body) inspection. After that, a protective film was placed on the polyimide resin layer, and 23 glass plates with a thickness of 2.8 mm were stacked and a load was applied, and placed in an atmosphere at a temperature of 40°C and a relative humidity of 80% for 5 days. Next, the protective film was peeled off, and the surface of the polyimide resin layer was inspected for defects (foreign objects) on the surface of the polyimide resin layer again using an optical inspection device made by Orbotech. By comparing the defect distribution of the optical inspection device made by Orbotech before and after the protective film is laminated, it is confirmed whether the foreign matter on the polyimide resin layer before the laminating still remains after the protective film is peeled off, and the foreign matter remains afterwards. Use an optical microscope and a scanning electron microscope (SEM) to observe the surface of foreign objects. By comparing the image of the optical microscope with the image of the scanning electron microscope, it is judged whether it is an embedded foreign body.

(關於長期保存之評估) 於以貼合保護膜，對貼合面施加荷重之狀態保存之情形時，實施聚醯亞胺樹脂層表面是否產生黏著劑殘留或損傷之確認。各例中，各準備3片長期保存試驗用積層基板。各例中，於設置保護膜前，使用Orbotech公司製光學式檢查裝置，預先取得聚醯亞胺樹脂層表面存在之缺陷之位置資訊及圖像。接著，於聚醯亞胺樹脂層上設置保護膜，以對各例中獲得之積層基板之保護膜上，施加16 g/cm2 之荷重之狀態，於溫度40°C、相對濕度80%之氛圍中放置5天。其後，於常溫、常壓之環境下取出，並以施加16 g/cm2 之荷重之狀態放置。於放置在溫度40°C、相對濕度80%之氛圍之期間、與常溫、常壓下取出後再放置之期間之和為2個月、4個月、6個月之各時期，自貼合有保護膜之1片積層基板去除荷重，剝離保護膜，再次使用Orbotech公司製光學式檢查裝置，取得聚醯亞胺樹脂層表面存在之缺陷之位置資訊及圖像。預先定義顯示黏著劑殘留或損傷之圖像，且於比較圖像時，參考顯示黏著劑殘留或損傷之圖像，評估有無黏著劑殘留或損傷。 將設置保護膜前後之圖像進行比較，評估有無黏著劑殘留或損傷。(Evaluation of long-term storage) When storing in a state where a protective film is attached and a load is applied to the attached surface, confirm whether there is adhesive residue or damage on the surface of the polyimide resin layer. In each case, 3 laminated substrates for long-term storage tests were prepared. In each case, before installing the protective film, an optical inspection device made by Orbotech was used to obtain the position information and images of the defects on the surface of the polyimide resin layer in advance. Next, a protective film was placed on the polyimide resin layer to apply a load of 16 g/cm 2 to the protective film of the laminated substrate obtained in each example at a temperature of 40°C and a relative humidity of 80%. Leave it in the atmosphere for 5 days. After that, it was taken out under normal temperature and normal pressure, and placed in a state of applying a load of 16 g/cm 2. During the period of placing in an atmosphere with a temperature of 40°C and a relative humidity of 80%, the sum of the period of being taken out and placed under normal temperature and normal pressure is 2 months, 4 months, and 6 months. Self-adhesive Remove the load on a laminated substrate with a protective film, peel off the protective film, and again use an optical inspection device made by Orbotech to obtain location information and images of defects on the surface of the polyimide resin layer. Predefine the image showing adhesive residue or damage, and when comparing images, refer to the image showing adhesive residue or damage to evaluate whether there is adhesive residue or damage. Compare the images before and after setting the protective film to evaluate whether there is adhesive residue or damage.

以下，針對例1～16進行說明。 ＜例1＞ (硬化性矽酮之調製) 於1L之燒瓶中，加入三乙氧基甲基矽烷(179 g)、甲苯(300 g)、乙酸(5 g)，將混合物以25°C攪拌20分鐘後，進而加熱至60°C，使之反應12小時。將所得之反應粗液冷卻至25°C後，用水(300 g)，將反應粗液清洗3次。 於清洗後之反應粗液加入氯化三甲基矽烷(70 g)，將混合物以25°C攪拌20分鐘後，進而加熱至50°C，使之反應12小時。將所得之反應粗液冷卻至25°C後，用水(300 g)，將反應粗液清洗3次。 自清洗後之反應粗液減壓餾去甲苯，設為漿體狀態後，以真空乾燥機乾燥一晚上，藉此獲得白色有機聚矽氧烷化合物即硬化性矽酮1。硬化性矽酮1之T單位之個數：M單位之個數=87:13(莫耳比)。 另，M單位意指以(R)3 SiO1/2 表示之1官能有機矽烷氧基單位。T單位意指以RSiO3/2 (R表示氫原子或有機基)表示之3官能有機矽烷氧基單位。Hereinafter, examples 1 to 16 will be described. <Example 1> (Preparation of curable silicone) In a 1L flask, add triethoxymethylsilane (179 g), toluene (300 g), and acetic acid (5 g), and stir the mixture at 25°C After 20 minutes, it was further heated to 60°C and reacted for 12 hours. After the obtained crude reaction liquid was cooled to 25°C, the crude reaction liquid was washed 3 times with water (300 g). Trimethylsilyl chloride (70 g) was added to the washed crude reaction solution, and the mixture was stirred at 25°C for 20 minutes, and then heated to 50°C to react for 12 hours. After the obtained crude reaction liquid was cooled to 25°C, the crude reaction liquid was washed 3 times with water (300 g). Toluene was removed under reduced pressure from the reaction crude liquid after washing, and after it was put into a slurry state, it was dried in a vacuum dryer overnight, thereby obtaining a white organopolysiloxane compound, that is, curable silicone 1. The number of T units of the sclerosing silicone 1: the number of M units=87:13 (mole ratio). In addition, the M unit means a monofunctional organosilicon alkoxy unit represented by (R) 3 SiO 1/2. The T unit means a trifunctional organosilicon alkoxy unit represented by RSiO 3/2 (R represents a hydrogen atom or an organic group).

(硬化性組合物之調製) 將硬化性矽酮1與作為溶媒之己烷混合，進而添加作為金屬化合物之2-乙基己酸鉍(III)。溶媒量以固體部分濃度為50質量%之方式調整。又，金屬化合物之添加量以金屬元素相對於樹脂100質量部為0.01質量部之方式調整。藉由使用孔徑為0.45 μm之過濾器過濾所得之混合液，而獲得硬化性組合物。(Preparation of curable composition) The curable silicone 1 is mixed with hexane as a solvent, and bismuth (III) 2-ethylhexanoate as a metal compound is added. The amount of solvent is adjusted so that the solid content concentration is 50% by mass. In addition, the addition amount of the metal compound was adjusted so that the metal element was 0.01 parts by mass relative to 100 parts by mass of the resin. The curable composition was obtained by filtering the resulting mixed liquid with a filter with a pore size of 0.45 μm.

(積層基板之製作) 將調製之硬化性組合物塗佈於厚度0.015 mm之聚醯亞胺薄膜(東洋紡股份有限公司製，商品名「XENOMAX」)，使用加熱板以140°C加熱10分鐘，藉此形成矽酮樹脂層。矽酮樹脂層之厚度為10 μm。 接著，將以水系玻璃清洗劑(Parkercorp股份有限公司製，「PK-LGC213」)清洗後，以純水清洗之200×200 mm，厚度為0.05 mm之玻璃板「AN100」(支持基材)置於矽酮樹脂層上，使用貼合裝置使之貼合，而製作積層體。 接著，將所得之積層體於氮氣氛圍下以500°C加熱30分。其後，實施空氣吹送，將細小之塵埃自聚醯亞胺薄膜之表面去除。 將保護膜1貼合於所得之積層體之聚醯亞胺薄膜側，獲得積層基板。作為使用之保護膜1，使用厚度為55 μm之Panac股份有限公司 Panaprotect(註冊商標)ETK50B(商品名)。保護膜1具有基材(厚度50 μm，PET薄膜)與黏著層。(Production of multilayer substrates) The prepared curable composition is applied to a polyimide film (manufactured by Toyobo Co., Ltd., trade name "XENOMAX") with a thickness of 0.015 mm, and heated at 140°C for 10 minutes using a hot plate to form a silicone resin Floor. The thickness of the silicone resin layer is 10 μm. Next, after cleaning with a water-based glass cleaner (Parkercorp Co., Ltd., "PK-LGC213"), a 200×200 mm glass plate with a thickness of 0.05 mm, "AN100" (supporting base material), is cleaned with pure water. Laminate the silicone resin layer using a laminating device to produce a laminate. Next, the resulting laminate was heated at 500°C for 30 minutes in a nitrogen atmosphere. After that, air blowing was performed to remove fine dust from the surface of the polyimide film. The protective film 1 was bonded to the polyimide film side of the obtained laminate to obtain a laminate substrate. As the protective film 1 used, Panac Co., Ltd. Panaprotect (registered trademark) ETK50B (trade name) with a thickness of 55 μm was used. The protective film 1 has a base material (thickness 50 μm, PET film) and an adhesive layer.

＜例2～16＞ 除變更保護膜之種類以外，根據與例1同樣之程序，獲得例2～例16之積層基板。 另，例2中，作為保護膜2，使用厚度為65 μm之Panac股份有限公司 Panaprotect(註冊商標)PX50T01A15(商品名)。保護膜2具有基材(厚度為50 μm，PET薄膜)與黏著層。 例3中，作為保護膜3，使用厚度為55 μm之藤森工業股份有限公司 Mastac(註冊商標)PC-751(商品名)。保護膜3具有基材(厚度為50 μm，PET薄膜)與黏著層。 例4中，作為保護膜4，使用具有厚度為65 μm之基材(PET薄膜)與黏著層之薄膜。 例5中，作為保護膜5，使用厚度為70 μm之Sun-A.Kaken股份有限公司 PAC-3-70(商品名)。保護膜5為LDPE(低密度聚乙烯)薄膜與乙烯-乙酸乙烯酯共聚物層之共擠出薄膜。＜Example 2～16＞ Except for changing the type of the protective film, according to the same procedure as in Example 1, the laminated substrates of Examples 2 to 16 were obtained. In addition, in Example 2, as the protective film 2, Panac Co., Ltd. Panaprotect (registered trademark) PX50T01A15 (trade name) with a thickness of 65 μm was used. The protective film 2 has a base material (50 μm in thickness, PET film) and an adhesive layer. In Example 3, as the protective film 3, Fujimori Industrial Co., Ltd. Mastac (registered trademark) PC-751 (trade name) having a thickness of 55 μm was used. The protective film 3 has a base material (50 μm in thickness, PET film) and an adhesive layer. In Example 4, as the protective film 4, a film having a base material (PET film) with a thickness of 65 μm and an adhesive layer was used. In Example 5, as the protective film 5, Sun-A. Kaken Co., Ltd. PAC-3-70 (trade name) with a thickness of 70 μm was used. The protective film 5 is a co-extruded film of an LDPE (low density polyethylene) film and an ethylene-vinyl acetate copolymer layer.

例6中，作為保護膜6，使用厚度為30 μm之Futamura(二村)化學股份有限公司 FSA(註冊商標)010M(商品名)。保護膜6為將雙軸延伸聚丙烯(OPP)作為基材(厚度為30 μm)之自黏性保護膜。 例7中，作為保護膜7，使用厚度為57 μm之Panac股份有限公司 Panaprotect(註冊商標)ST50(商品名)。保護膜7具有基材(厚度為50 μm、PET薄膜)與黏著層。 例8中，作為保護膜8，使用厚度為80 μm之Panac股份有限公司 Panaprotect(註冊商標)GC50(商品名)。保護膜8具有基材(厚度為50 μm、PET薄膜)與黏著層。 例9中，作為保護膜9，使用厚度為63 μm之Panac股份有限公司 Panaprotect(註冊商標)GS50(商品名)。保護膜9具有基材(厚度50 μm、PET薄膜)與黏著層。 例10中，作為保護膜10，使用厚度為60 μm之Panac股份有限公司 Panaprotect(註冊商標)GN50(商品名)。保護膜10具有基材(厚度為50 μm、PET薄膜)與黏著層。In Example 6, as the protective film 6, Futamura (Futamura) Chemical Co., Ltd. FSA (registered trademark) 010M (trade name) with a thickness of 30 μm was used. The protective film 6 is a self-adhesive protective film using biaxially stretched polypropylene (OPP) as a base material (thickness of 30 μm). In Example 7, as the protective film 7, Panaprotect (registered trademark) ST50 (trade name) of Panac Co., Ltd. having a thickness of 57 μm was used. The protective film 7 has a base material (50 μm in thickness, PET film) and an adhesive layer. In Example 8, as the protective film 8, Panac Co., Ltd. Panaprotect (registered trademark) GC50 (trade name) with a thickness of 80 μm was used. The protective film 8 has a base material (50 μm in thickness, PET film) and an adhesive layer. In Example 9, as the protective film 9, Panac Co., Ltd. Panaprotect (registered trademark) GS50 (trade name) with a thickness of 63 μm was used. The protective film 9 has a base material (thickness 50 μm, PET film) and an adhesive layer. In Example 10, as the protective film 10, Panac Co., Ltd. Panaprotect (registered trademark) GN50 (trade name) with a thickness of 60 μm was used. The protective film 10 has a base material (50 μm in thickness, PET film) and an adhesive layer.

例11中，作為保護膜11，使用厚度為60 μm之Sun-A.Kaken股份有限公司 JA16F(商品名)。保護膜11具有基材(LDPE薄膜)與黏著層。 例12中，作為保護膜12，使用厚度為60 μm之Sun-A.Kaken股份有限公司 Y16F(商品名)。保護膜12具有基材(LDPE薄膜)與黏著層。 例13中，作為保護膜13，使用厚度為74 μm之Sun-A.Kaken股份有限公司 P27(商品名)。保護膜13具有基材(PE薄膜)與黏著層。 例14中，作為保護膜14，使用厚度為50 μm之Sun-A.Kaken股份有限公司 B35(商品名)。保護膜14具有基材(PE薄膜)與黏著層。 例15中，作為保護膜15，使用厚度為50 μm之原紙漿襯紙。保護膜15不具有黏著層。 例16中，作為保護膜16，使用厚度為50 μm之PET薄膜。保護膜16不具有黏著層。In Example 11, as the protective film 11, Sun-A. Kaken Co., Ltd. JA16F (trade name) having a thickness of 60 μm was used. The protective film 11 has a base material (LDPE film) and an adhesive layer. In Example 12, as the protective film 12, Sun-A. Kaken Co., Ltd. Y16F (trade name) with a thickness of 60 μm was used. The protective film 12 has a base material (LDPE film) and an adhesive layer. In Example 13, as the protective film 13, Sun-A. Kaken Co., Ltd. P27 (trade name) having a thickness of 74 μm was used. The protective film 13 has a base material (PE film) and an adhesive layer. In Example 14, as the protective film 14, Sun-A. Kaken Co., Ltd. B35 (trade name) having a thickness of 50 μm was used. The protective film 14 has a base material (PE film) and an adhesive layer. In Example 15, as the protective film 15, a base pulp liner with a thickness of 50 μm was used. The protective film 15 does not have an adhesive layer. In Example 16, as the protective film 16, a PET film with a thickness of 50 μm was used. The protective film 16 does not have an adhesive layer.

各例之積層基板之第1密著力及第2密著力彙總顯示於表1及表2中。各密著力之測定方法如上所述。 表1及表2中之「黏著劑」欄位表示保護膜中之黏著層中之黏著劑之種類，「丙烯酸系」意指黏著劑為丙烯酸系黏著劑，「矽酮系」意指黏著劑為矽酮系黏著劑。The first adhesion force and the second adhesion force of the laminated substrate of each example are collectively shown in Table 1 and Table 2. The measuring method of each adhesion force is as described above. The "adhesive" column in Table 1 and Table 2 indicates the type of adhesive in the adhesive layer of the protective film. "Acrylic" means that the adhesive is an acrylic adhesive, and "silicone" means an adhesive It is a silicone adhesive.

[表1] 表1 例1 例2 例3 例4 例5 例6 例7 例8 保護膜 基材之材料 PET PET PET PET LDPE OPP PET PET 保護膜之 厚度(μm) 55 65 55 65 70 30 57 80 黏著劑 丙烯酸系 矽酮系 丙烯酸系 矽酮系 — — 丙烯酸系 丙烯酸系 評估 第1密著力(N/10 mm) 0.120 0.160 0.096 0.004 0.142 0.064 0.200 0.400 第2密著力(N/10 mm) 0.099 0.114 0.073 0.072 0.128 0.072 0.122 0.212 外周部異物 無 無 無 無 無 無 無 無 黏著劑殘留 無 無 無 無 無 無 有 有 損傷 無 無 無 無 無 無 無 無 支持基材 破損 無 無 無 無 無 無 無 無 耐熱試驗 ○ ○ ○ ○ ○ ○ — — 埋沒異物 — — — 有 無 無 — — [Table 1] Table 1 example 1 Example 2 Example 3 Example 4 Example 5 Example 6 Example 7 Example 8 Protective film Substrate material PET PET PET PET LDPE OPP PET PET Thickness of protective film (μm) 55 65 55 65 70 30 57 80 Adhesive Acrylic Silicone series Acrylic Silicone series — — Acrylic Acrylic Assessment 1st adhesion force (N/10 mm) 0.120 0.160 0.096 0.004 0.142 0.064 0.200 0.400 2nd adhesion force (N/10 mm) 0.099 0.114 0.073 0.072 0.128 0.072 0.122 0.212 Peripheral foreign body no no no no no no no no Adhesive residue no no no no no no Have Have damage no no no no no no no no Support broken substrate no no no no no no no no Heat resistance test ○ ○ ○ ○ ○ ○ — — Buried foreign body — — — Have no no — —

[表2] 表2 例9 例10 例11 例12 例13 例14 例15 例16 保護膜 基材之材料 PET PET LDPE LDPE PE PE 原紙漿襯紙 PET 保護膜之 厚度(μm) 63 60 60 60 74 50 50 50 黏著劑 丙烯酸系 丙烯酸系 丙烯酸系 丙烯酸系 丙烯酸系 丙烯酸系 — — 評估 第1密著力(N/10 mm) 1.200 0.560 0.406 0.554 1.968 0.793 0.003 0.005 第2密著力(N/10 mm) 0.687 0.32 0.271 0.640 1.600 0.212 0.004 0.01 外周部異物 無 無 無 無 無 無 有 有 黏著劑殘留 有 有 有 有 有 有 無 無 損傷 無 無 無 無 無 無 有 有 支持基材 破損 無 無 無 無 有 無 無 無 耐熱試驗 — — — — — — — — 埋沒異物 — — — — — — — — [Table 2] Table 2 Example 9 Example 10 Example 11 Example 12 Example 13 Example 14 Example 15 Example 16 Protective film Substrate material PET PET LDPE LDPE PE PE Paper pulp liner PET Thickness of protective film (μm) 63 60 60 60 74 50 50 50 Adhesive Acrylic Acrylic Acrylic Acrylic Acrylic Acrylic — — Assessment 1st adhesion force (N/10 mm) 1.200 0.560 0.406 0.554 1.968 0.793 0.003 0.005 2nd adhesion force (N/10 mm) 0.687 0.32 0.271 0.640 1.600 0.212 0.004 0.01 Peripheral foreign body no no no no no no Have Have Adhesive residue Have Have Have Have Have Have no no damage no no no no no no Have Have Support broken substrate no no no no Have no no no Heat resistance test — — — — — — — — Buried foreign body — — — — — — — —

＜評估結果之總結＞ 如上述表1及表2所示，滿足特定要件之例1～6中，獲得期望之效果。 另，例1～6中，由於保護膜與聚醯亞胺樹脂層之第1密著力為0.001 N/10 mm以上且0.17 N/10 mm以下，故即使於大氣環境中進行輸送，亦不會產生保護膜與聚醯亞胺樹脂層之剝離，且未確認到聚醯亞胺樹脂層之端部缺陷增加。再者，由於例1～6中，支持基材與保護膜之第2密著力F2 為0.05 N/10 mm≦F2 ≦(F1 (N/10 mm)+0.3 N/10 mm)，故保護膜剝離時，可順利地剝離，不會對支持基材產生損傷。 另，例4～6中，將保護膜切成100 mm×100 mm之大小，以與黏著面相反側對向之方式對折。接著，使用玻璃基板，將16 g/cm2 之荷重施加至對折者。並以施加荷重之狀態放置30分後，取下玻璃基板。且，確認保護膜復原至何種程度。例5、6中，仍維持彎折狀態(0°)，但例4中，保護膜復原至某程度成為90°。因此，例4中，保護膜之復原力相對強，不易追隨異物而變形，故推測為能將異物推壓至聚醯亞胺樹脂層。 又，例5、6中，實施長期保存試驗，但於長期保存2個月、4個月、6個月後之任一保存期間，皆未發現黏著劑殘留、損傷。<Summary of Evaluation Results> As shown in Table 1 and Table 2, the desired effects were obtained in Examples 1 to 6 that satisfy the specified requirements. In addition, in Examples 1 to 6, since the first adhesive force between the protective film and the polyimide resin layer is 0.001 N/10 mm or more and 0.17 N/10 mm or less, it will not be transported in an atmospheric environment. Peeling of the protective film and the polyimide resin layer occurred, and no increase in end defects of the polyimide resin layer was confirmed. Furthermore, since in Examples 1 to 6, the second adhesion force F 2 between the supporting substrate and the protective film is 0.05 N/10 mm≦F 2 ≦(F 1 (N/10 mm)+0.3 N/10 mm), Therefore, when the protective film is peeled off, it can be peeled off smoothly without causing damage to the supporting substrate. In addition, in Examples 4 to 6, the protective film was cut into a size of 100 mm×100 mm, and folded in half facing the opposite side of the adhesive surface. Next, using a glass substrate, a load of 16 g/cm 2 is applied to the person who is folded in half. After placing the load for 30 minutes, remove the glass substrate. And, confirm how much the protective film has recovered. In Examples 5 and 6, the bent state (0°) was still maintained, but in Example 4, the protective film was restored to a certain degree and became 90°. Therefore, in Example 4, the protective film has relatively strong resilience and is not easy to follow the foreign matter and deform, so it is presumed that it can push the foreign matter to the polyimide resin layer. In addition, in Examples 5 and 6, the long-term storage test was carried out, but no adhesive residue or damage was found during any storage period after the long-term storage for 2 months, 4 months, and 6 months.

本申請案係基於2019年6月6日申請之日本專利申請案2019-106053者，其之內容以引用之方式併入於本文中。This application is based on the Japanese patent application 2019-106053 filed on June 6, 2019, the content of which is incorporated herein by reference.

10:積層基板 12:支持基材 12a:表面 12b:背面 12c:外緣部 13:矽酮樹脂層 13a:表面 14:聚醯亞胺樹脂層 14a:表面 16:保護膜 18:基材 19:密著層 20:捆包體 22:托板 24:底板 24a:表面 26:背板 26a:表面 D:異物 β:角度10: Multilayer substrate 12: Support substrate 12a: surface 12b: back 12c: Outer edge 13: Silicone resin layer 13a: surface 14: Polyimide resin layer 14a: surface 16: Protective film 18: Substrate 19: Adhesive layer 20: Packing body 22: Pallet 24: bottom plate 24a: surface 26: backplane 26a: surface D: Foreign body β: Angle

圖1係模式性顯示本發明之實施形態之積層基板之第1例之俯視圖。 圖2係模式性顯示本發明之實施形態之積層基板之第1例之剖視圖。 圖3係模式性顯示本發明之實施形態之積層基板之第1例之保護膜之剖視圖。 圖4係模式性顯示本發明之實施形態之積層基板之第2例之俯視圖。 圖5係模式性顯示本發明之實施形態之積層基板之第3例之剖視圖。 圖6係模式性顯示本發明之實施形態之捆包體之一例之側視圖。 圖7係模式性說明本發明之實施形態之積層基板中埋設物的產生之剖視圖。 圖8係模式性說明本發明之實施形態之積層基板中埋設物的產生之剖視圖。 圖9係模式性說明本發明之實施形態之積層基板中埋設物的產生之剖視圖。 圖10係顯示本發明之實施形態之積層基板中之埋設物之一例之SEM(Scanning Electron Microscope：掃描電子顯微鏡)像。Fig. 1 is a plan view schematically showing the first example of the multilayer substrate of the embodiment of the present invention. Fig. 2 is a cross-sectional view schematically showing the first example of the multilayer substrate of the embodiment of the present invention. Fig. 3 is a cross-sectional view schematically showing the protective film of the first example of the multilayer substrate of the embodiment of the present invention. Fig. 4 is a plan view schematically showing the second example of the multilayer substrate of the embodiment of the present invention. Fig. 5 is a cross-sectional view schematically showing a third example of the multilayer substrate of the embodiment of the present invention. Fig. 6 is a side view schematically showing an example of the packing body of the embodiment of the present invention. FIG. 7 is a cross-sectional view schematically illustrating the generation of embedded objects in the multilayer substrate according to the embodiment of the present invention. FIG. 8 is a cross-sectional view schematically illustrating the generation of embedded objects in the multilayer substrate according to the embodiment of the present invention. FIG. 9 is a cross-sectional view schematically illustrating the generation of embedded objects in the multilayer substrate according to the embodiment of the present invention. FIG. 10 is an SEM (Scanning Electron Microscope) image showing an example of the embedded object in the laminated substrate of the embodiment of the present invention.

10:積層基板 10: Multilayer substrate

12:支持基材 12: Support substrate

12a:表面 12a: surface

12c:外緣部 12c: Outer edge

14:聚醯亞胺樹脂層 14: Polyimide resin layer

14a:表面 14a: surface

16:保護膜 16: Protective film

18:基材 18: Substrate

19:密著層 19: Adhesive layer

Claims (11)

一種積層基板，其係於玻璃製之支持基材上，積層有聚醯亞胺樹脂層、與覆蓋上述聚醯亞胺樹脂層之保護膜者，且 將上述聚醯亞胺樹脂層與上述保護膜之第1密著力設為F1 ，將上述支持基材與上述保護膜之第2密著力設為F2 時， 上述第1密著力F1 為0.001 N/10 mm≦F1 ≦0.17 N/10 mm， 上述第2密著力F2 為0.05 N/10 mm≦F2 ≦(F1 (N/10 mm)+0.3 N/10 mm)。A laminated substrate, which is on a supporting substrate made of glass, laminated with a polyimide resin layer, and a protective film covering the polyimide resin layer, and combining the polyimide resin layer and the protective film When the first adhesion force of the film is F 1 , and the second adhesion force of the support substrate and the protective film is F 2 , the first adhesion force F 1 is 0.001 N/10 mm≦F 1 ≦0.17 N /10 mm, the above-mentioned second adhesion force F 2 is 0.05 N/10 mm≦F 2 ≦(F 1 (N/10 mm)+0.3 N/10 mm). 如請求項1之積層基板，其中上述保護膜之大小為上述支持基材之大小以上。The laminated substrate of claim 1, wherein the size of the protective film is greater than the size of the supporting base material. 如請求項1或2之積層基板，其中上述保護膜之厚度為20 μm以上。The multilayer substrate of claim 1 or 2, wherein the thickness of the protective film is 20 μm or more. 如請求項1至3中任一項之積層基板，其中上述保護膜具有基材、及積層於上述基材且與上述聚醯亞胺樹脂層相接之密著層，上述基材由聚乙烯構成。The laminated substrate according to any one of claims 1 to 3, wherein the protective film has a base material and an adhesion layer laminated on the base material and in contact with the polyimide resin layer, and the base material is made of polyethylene constitute. 如請求項1至4中任一項之積層基板，其中上述支持基材與上述聚醯亞胺樹脂層之密著力大於上述第1密著力及上述第2密著力之任一者。The laminated substrate according to any one of claims 1 to 4, wherein the adhesion force of the support base material and the polyimide resin layer is greater than any one of the first adhesion force and the second adhesion force. 如請求項1至5中任一項之積層基板，其中於上述支持基材與上述聚醯亞胺樹脂層間，設置有矽烷偶合劑層。The laminated substrate according to any one of claims 1 to 5, wherein a silane coupling agent layer is provided between the supporting base material and the polyimide resin layer. 如請求項1至5中任一項之積層基板，其中於上述支持基材與上述聚醯亞胺樹脂層間，設置有矽酮樹脂層。The laminated substrate according to any one of claims 1 to 5, wherein a silicone resin layer is provided between the support base material and the polyimide resin layer. 一種捆包體，其具有托板、及以複數片裝載於上述托板之請求項1至7中任一項之積層基板。A package body has a pallet and a plurality of laminated substrates loaded on the pallet in any one of claims 1 to 7. 如請求項8之捆包體，其中複數片上述積層基板以相互施加荷重之狀態裝載於上述托板。The package of claim 8, wherein a plurality of the above-mentioned laminated substrates are loaded on the above-mentioned pallet in a state where a load is applied to each other. 如請求項8或9之捆包體，其中上述托板具有底板、及立設於上述底板之背板，且 上述積層基板以使上述支持基材朝向上述背板之表面傾斜之狀態裝載於上述托板。Such as the package body of claim 8 or 9, wherein the pallet has a bottom plate and a back plate erected on the bottom plate, and The laminated substrate is mounted on the pallet in a state where the supporting base material is inclined toward the surface of the backing plate. 如請求項8至10中任一項之捆包體，其中上述積層基板之大小係短邊為850 mm以上，長邊為1100 mm以上。Such as the package of any one of claims 8 to 10, wherein the size of the laminated substrate is 850 mm or more on the short side and 1100 mm or more on the long side.
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