WO2019235217A1 - Procédé de production de produit d'étanchéité durci - Google Patents

Procédé de production de produit d'étanchéité durci Download PDF

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Publication number
WO2019235217A1
WO2019235217A1 PCT/JP2019/020190 JP2019020190W WO2019235217A1 WO 2019235217 A1 WO2019235217 A1 WO 2019235217A1 JP 2019020190 W JP2019020190 W JP 2019020190W WO 2019235217 A1 WO2019235217 A1 WO 2019235217A1
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WO
WIPO (PCT)
Prior art keywords
expandable
pressure
sensitive adhesive
layer
adhesive layer
Prior art date
Application number
PCT/JP2019/020190
Other languages
English (en)
Japanese (ja)
Inventor
忠知 山田
真也 田久
Original Assignee
リンテック株式会社
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by リンテック株式会社 filed Critical リンテック株式会社
Priority to JP2020523609A priority Critical patent/JP7267272B2/ja
Priority to KR1020207035077A priority patent/KR102727202B1/ko
Priority to CN201980038938.3A priority patent/CN112262459A/zh
Publication of WO2019235217A1 publication Critical patent/WO2019235217A1/fr

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    • C—CHEMISTRY; METALLURGY
    • C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09J—ADHESIVES; NON-MECHANICAL ASPECTS OF ADHESIVE PROCESSES IN GENERAL; ADHESIVE PROCESSES NOT PROVIDED FOR ELSEWHERE; USE OF MATERIALS AS ADHESIVES
    • C09J201/00—Adhesives based on unspecified macromolecular compounds
    • C—CHEMISTRY; METALLURGY
    • C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09J—ADHESIVES; NON-MECHANICAL ASPECTS OF ADHESIVE PROCESSES IN GENERAL; ADHESIVE PROCESSES NOT PROVIDED FOR ELSEWHERE; USE OF MATERIALS AS ADHESIVES
    • C09J7/00—Adhesives in the form of films or foils
    • C09J7/20—Adhesives in the form of films or foils characterised by their carriers
    • C—CHEMISTRY; METALLURGY
    • C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09J—ADHESIVES; NON-MECHANICAL ASPECTS OF ADHESIVE PROCESSES IN GENERAL; ADHESIVE PROCESSES NOT PROVIDED FOR ELSEWHERE; USE OF MATERIALS AS ADHESIVES
    • C09J7/00—Adhesives in the form of films or foils
    • C09J7/30—Adhesives in the form of films or foils characterised by the adhesive composition
    • C09J7/38—Pressure-sensitive adhesives [PSA]
    • 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
    • H01L21/02—Manufacture or treatment of semiconductor devices or of parts thereof
    • H01L21/04—Manufacture or treatment of semiconductor devices or of parts thereof the devices having potential barriers, e.g. a PN junction, depletion layer or carrier concentration layer
    • H01L21/50—Assembly of semiconductor devices using processes or apparatus not provided for in a single one of the subgroups H01L21/06 - H01L21/326, e.g. sealing of a cap to a base of a container
    • H01L21/56—Encapsulations, e.g. encapsulation layers, coatings
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
    • H01L23/00—Details of semiconductor or other solid state devices
    • H01L23/28—Encapsulations, e.g. encapsulating layers, coatings, e.g. for protection
    • H01L23/29—Encapsulations, e.g. encapsulating layers, coatings, e.g. for protection characterised by the material, e.g. carbon
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
    • H01L23/00—Details of semiconductor or other solid state devices
    • H01L23/28—Encapsulations, e.g. encapsulating layers, coatings, e.g. for protection
    • H01L23/31—Encapsulations, e.g. encapsulating layers, coatings, e.g. for protection characterised by the arrangement or shape
    • C—CHEMISTRY; METALLURGY
    • C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09J—ADHESIVES; NON-MECHANICAL ASPECTS OF ADHESIVE PROCESSES IN GENERAL; ADHESIVE PROCESSES NOT PROVIDED FOR ELSEWHERE; USE OF MATERIALS AS ADHESIVES
    • C09J2203/00—Applications of adhesives in processes or use of adhesives in the form of films or foils
    • C09J2203/326—Applications of adhesives in processes or use of adhesives in the form of films or foils for bonding electronic components such as wafers, chips or semiconductors
    • C—CHEMISTRY; METALLURGY
    • C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09J—ADHESIVES; NON-MECHANICAL ASPECTS OF ADHESIVE PROCESSES IN GENERAL; ADHESIVE PROCESSES NOT PROVIDED FOR ELSEWHERE; USE OF MATERIALS AS ADHESIVES
    • C09J2301/00—Additional features of adhesives in the form of films or foils
    • C09J2301/10—Additional features of adhesives in the form of films or foils characterized by the structural features of the adhesive tape or sheet
    • C09J2301/12—Additional features of adhesives in the form of films or foils characterized by the structural features of the adhesive tape or sheet by the arrangement of layers
    • C09J2301/124—Additional features of adhesives in the form of films or foils characterized by the structural features of the adhesive tape or sheet by the arrangement of layers the adhesive layer being present on both sides of the carrier, e.g. double-sided adhesive tape
    • C—CHEMISTRY; METALLURGY
    • C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09J—ADHESIVES; NON-MECHANICAL ASPECTS OF ADHESIVE PROCESSES IN GENERAL; ADHESIVE PROCESSES NOT PROVIDED FOR ELSEWHERE; USE OF MATERIALS AS ADHESIVES
    • C09J2301/00—Additional features of adhesives in the form of films or foils
    • C09J2301/30—Additional features of adhesives in the form of films or foils characterized by the chemical, physicochemical or physical properties of the adhesive or the carrier
    • C09J2301/312—Additional features of adhesives in the form of films or foils characterized by the chemical, physicochemical or physical properties of the adhesive or the carrier parameters being the characterizing feature

Definitions

  • the present invention relates to a method for producing a cured encapsulant.
  • the pressure-sensitive adhesive sheet is used not only for semi-permanently fixing members but also for temporarily fixing the target members when processing or inspecting building materials, interior materials, electronic parts, etc. There is a case.
  • Such a pressure-sensitive adhesive sheet for temporarily fixing is required to satisfy both adhesiveness at the time of use and peelability after use.
  • Patent Document 1 discloses a heat-peelable pressure-sensitive adhesive sheet for temporary fixing at the time of cutting an electronic component, in which a heat-expandable pressure-sensitive adhesive layer containing heat-expandable microspheres is provided on at least one surface of a substrate. ing.
  • This heat-peelable pressure-sensitive adhesive sheet adjusts the maximum particle diameter of the heat-expandable microspheres with respect to the thickness of the heat-expandable pressure-sensitive adhesive layer, and calculates the centerline average roughness of the surface of the heat-expandable pressure-sensitive adhesive layer before heating. It is adjusted to 0.4 ⁇ m or less.
  • the heat-peelable pressure-sensitive adhesive sheet can sufficiently secure a bonding area with an adherend when an electronic component is cut, it can exhibit adhesiveness that can prevent adhesion failure such as chip jumping, Then, after use, there is a description that if the thermally expandable microspheres are expanded by heating, the contact area with the adherend can be reduced and can be easily peeled off.
  • FOWLP Fean out Wafer Level Package
  • FOWLP provides a rewiring layer on the surface of a semiconductor chip side of a hardened sealing body formed by sealing a plurality of semiconductor chips arranged at a predetermined interval with a sealing material, and soldering is performed via the rewiring layer.
  • FOWLP can be applied to an application where the number of terminals is larger than the area of the semiconductor chip because the terminals, which are solder balls, can be expanded to the outside of the semiconductor chip (Fan out).
  • FOWLP is a method in which a circuit surface of a semiconductor chip is placed on an adhesive sheet, and a sealing resin having fluidity heated to around 100 ° C. is filled around the semiconductor chip, heated, and sealed. Forming a layer composed of resin or laminating a sealing resin film on a semiconductor chip, heating and laminating, and removing the adhesive sheet and exposing the semiconductor chip side In general, it is manufactured through a step of forming a redistribution layer and solder balls on the surface of the substrate.
  • a heat-peelable adhesive in which a thermally expandable adhesive layer containing thermally expandable microspheres is provided on a substrate. It is also possible to use a sheet.
  • the heat-expandable pressure-sensitive adhesive layer of the heat-peelable pressure-sensitive adhesive sheet described in Patent Document 1 contains heat-expandable microspheres, it has a sealing process, etc., compared to an adhesive layer that does not contain heat-expandable microspheres.
  • the decrease in adhesive strength during the processing and inspection is caused by the displacement of the semiconductor chip placed on the adhesive layer or the sealing resin invading at the bonding interface between the semiconductor chip and the adhesive sheet. This causes a problem such as resin adhering to the circuit surface.
  • the elastic modulus of the heat-expandable pressure-sensitive adhesive layer is generally adjusted to be low so that irregularities are easily formed on the surface during expansion of the heat-expandable microspheres. There is a concern that the semiconductor chip placed on the surface of the adhesive layer is likely to be displaced during the sealing process.
  • the above heat-peelable pressure-sensitive adhesive sheet when used, it is separated at the interface between the heat-expandable pressure-sensitive adhesive layer and the cured sealing material, and the above-mentioned double-sided pressure-sensitive adhesive sheet remains adhered to the support.
  • the double-sided PSA sheet is removed from the substrate, a part of the PSA layer of the PSA sheet may remain on the adherend. In such a case, it is necessary to perform a cleaning process of the support, which causes a reduction in productivity.
  • the device needs to be cleaned, which causes a decrease in productivity. That is, in the production of a cured encapsulated body, it is also required to suppress the contamination in the production environment, do not require a cleaning step, and improve productivity.
  • a sealing object when a sealing object is obtained by using a sealing material to obtain a cured sealing body, occurrence of positional deviation of the sealing object and adhesion of the sealing resin to the exposed surface of the sealing object It is an object of the present invention to provide a method for producing a cured encapsulant that can effectively suppress adverse effects and improve yield, and can suppress contamination in a production environment and improve productivity.
  • the present inventors include a base material provided with at least an inflatable base material layer containing inflatable particles and a non-inflatable base material layer. It has been found that the above-mentioned problems can be solved by using a pressure-sensitive adhesive sheet having a first pressure-sensitive adhesive layer and a second pressure-sensitive adhesive layer, which are non-intumescent pressure-sensitive adhesive layers, on both sides.
  • a substrate (Y) comprising at least an expandable substrate layer (Y1) containing expandable particles and a non-expandable substrate layer (Y2); On both surfaces of the base material (Y), the first pressure-sensitive adhesive layer (X1) and the second pressure-sensitive adhesive layer (X2), which are non-intumescent pressure-sensitive adhesive layers, By the expansion of the expandable particles, unevenness can occur on the adhesive surface of the first pressure-sensitive adhesive layer (X1), using a pressure-sensitive adhesive sheet, a method for producing a cured sealing body, A method for producing a cured encapsulant comprising the following steps (1) to (3).
  • Step (1) The process of sticking the adhesion surface of a 1st adhesive layer (X1) on a hard support body, and mounting a sealing target object on a part of adhesion surface of a 2nd adhesive layer (X2). .
  • Step (2) The sealing object and the adhesive surface of the second pressure-sensitive adhesive layer (X2) at least in the periphery of the sealing object are covered with a sealing material, and the sealing material is cured. And the process of obtaining the hardening sealing body formed by sealing the said sealing target object with the said sealing material.
  • Step (3) The expandable particles are expanded and the hard support and the first pressure-sensitive adhesive layer (X1) are stacked while the cured sealing body is laminated on the second pressure-sensitive adhesive layer (X2). Separating at the interface P.
  • the pressure-sensitive adhesive sheet has a first pressure-sensitive adhesive layer (X1) on the base material (Y) on the side of the expandable base material layer (Y1), and the base material (Y) has the non-expandable group.
  • the manufacturing method of the hardening sealing body as described in said [1] which has a said 2nd adhesive layer (X2) in the material layer (Y2) side.
  • the base material (Y) is a non-expandable base material provided on the expandable base material layer (Y1) and the first adhesive layer (X1) side of the expandable base material layer (Y1).
  • the storage elastic modulus E ′ of the non-expandable base layer (Y2-1) when the expandable particles expand is determined by the storage modulus of the non-expandable base layer (Y2-2) when the expandable particles expand.
  • the non-expandable base layer (Y2) is present at a position farther from the first pressure-sensitive adhesive layer (X1) than the expandable base layer (Y1), and the expandable base layer
  • the non-intumescent substrate layer (Y2) does not exist between the layer (Y1) and the first pressure-sensitive adhesive layer (X1),
  • the storage elastic modulus E ′ of the non-expandable base layer (Y2) when the expandable particles expand is the storage elastic modulus E of the expandable base layer (Y1) when the expandable particles expand.
  • the method for producing a cured sealed body of the present invention when obtaining a cured sealed body with a sealing material, the occurrence of positional deviation of the sealed object or the exposed surface of the sealed object. It is possible to effectively suppress adverse effects such as adhesion of the sealing resin to the substrate and improve the yield, and to suppress contamination in the manufacturing environment and improve productivity.
  • FIG. 6 is a schematic cross-sectional view in steps (1) to (3) of the method for manufacturing a semiconductor chip of the present invention.
  • the “treatment for expanding” for example, when the expandable particles are thermally expandable particles, a heat treatment for 3 minutes may be performed at the expansion start temperature (t) of the thermally expandable particles. .
  • the “active ingredient” refers to a component excluding a diluent solvent among components contained in a target composition.
  • the mass average molecular weight (Mw) is a value in terms of standard polystyrene measured by a gel permeation chromatography (GPC) method, specifically a value measured based on the method described in the examples.
  • (meth) acrylic acid indicates both “acrylic acid” and “methacrylic acid”, and the same applies to other similar terms.
  • the lower limit value and upper limit value which were described in steps can be combined independently, respectively.
  • the description “preferably 10 to 90, more preferably 30 to 60”, “preferable lower limit (10)” and “more preferable upper limit (60)” are combined to obtain “10 to 60”. You can also.
  • the method for producing a cured encapsulant of the present invention comprises an expandable base material layer (Y1) and a non-expandable base material layer (Y2) containing expandable particles. It has at least a base material (Y) and a first pressure-sensitive adhesive layer (X1) and a second pressure-sensitive adhesive layer (X2) that are non-expandable pressure-sensitive adhesive layers on both sides of the base material (Y).
  • This is a method for producing a cured encapsulant using an adhesive sheet, in which irregularities can occur on the adhesive surface of the first adhesive layer (X1) due to the expansion of the expandable particles.
  • the production method of the present invention includes the following steps (1) to (3).
  • -Process (1) The process of sticking the adhesion surface of a 1st adhesive layer (X1) on a hard support body, and mounting a sealing target object on a part of adhesion surface of a 2nd adhesive layer (X2). .
  • Step (2) The sealing object and the adhesive surface of the second pressure-sensitive adhesive layer (X2) at least in the periphery of the sealing object are covered with a sealing material, and the sealing material is cured. And the process of obtaining the hardening sealing body formed by sealing the said sealing target object with the said sealing material.
  • Step (3) The expandable particles are expanded and the hard support and the first pressure-sensitive adhesive layer (X1) are stacked while the cured sealing body is laminated on the second pressure-sensitive adhesive layer (X2). Separating at the interface P.
  • FIG. 1 is a schematic cross-sectional view of the pressure-sensitive adhesive sheet showing an example of the configuration of the pressure-sensitive adhesive sheet used in the production method of the present invention.
  • the pressure-sensitive adhesive sheet used in the production method of the present invention includes a base (Y) having at least an expandable base layer (Y1) and a non-expandable base layer (Y2) as shown in FIG.
  • the adhesive sheet 1a which has a 1st adhesive layer (X1) and a 2nd adhesive layer (X2) which are non-expandable adhesive layers on both surfaces of a material (Y), respectively is mentioned.
  • the base material (Y) which the adhesive sheet 1a shown to Fig.1 (a) has has the structure which the expandable base material layer (Y1) and the non-expandable base material layer (Y2) laminated
  • the base material (Y) may have a configuration other than this.
  • the base material (Y) of the pressure-sensitive adhesive sheet 1b shown in FIG. 1 (b) the first non-thermally expandable base material layer (Y2-1) and the first non-expandable base material layer (Y2-1) and 2
  • a release material may be further laminated on the pressure-sensitive adhesive surface of the first pressure-sensitive adhesive layer (X1) and the pressure-sensitive adhesive surface of the second pressure-sensitive adhesive layer (X2).
  • a structure in which a release material having a release treatment applied to both sides is laminated on one adhesive surface of the first adhesive layer (X1) and the second adhesive layer (X2) is wound in a roll shape. It is good.
  • These release materials are provided to protect the adhesive surfaces of the first adhesive layer (X1) and the second adhesive layer (X2), and are removed when the adhesive sheet is used.
  • the peeling force when peeling the release material laminated on the first pressure-sensitive adhesive layer (X1) and the second pressure-sensitive adhesive layer (X2) are laminated.
  • the adhesive sheet 1a is divided along with the two release materials and peeled off by pulling both release materials outward. This may cause a negative effect.
  • the release material laminated on the first pressure-sensitive adhesive layer (X1) and the release material laminated on the second pressure-sensitive adhesive layer (X2) have different peeling forces from the pressure-sensitive adhesive layer attached to each other. It is preferable to use two types of designed release materials.
  • the pressure-sensitive adhesive sheet used in the production method of the present invention is adjusted so that irregularities can be generated on the pressure-sensitive adhesive surface of the first pressure-sensitive adhesive layer (X1) by the expansion of the expandable particles.
  • a first pressure-sensitive adhesive layer (X1) that is a non-expandable pressure-sensitive adhesive layer is laminated on an expandable base material layer (Y1) containing expandable particles.
  • Y1 expandable base material layer
  • it has the structure which laminated
  • the adhesive surface of the first adhesive layer (X1) is affixed to a hard support.
  • the sealing object is placed on the adhesive surface of the second pressure-sensitive adhesive layer (X2).
  • step (2) the placed sealing object and Then, the second pressure-sensitive adhesive layer (X2) at the periphery of the object to be sealed is covered with a sealing material, and the sealing material is cured to form a cured sealing body.
  • step (3) when the expandable particles are expanded, the hard support and the first pressure-sensitive adhesive remain stacked on the second pressure-sensitive adhesive layer (X2). They are separated at the interface P with the agent layer (X1). That is, when separating from the hard support, the plurality of semiconductor chips are required to be held on the second pressure-sensitive adhesive layer (X2) of the pressure-sensitive adhesive sheet. Therefore, the pressure-sensitive adhesive surface of the second pressure-sensitive adhesive layer (X2) is suppressed from forming irregularities so that the adhesive force sufficient to hold the cured sealing body can be maintained by the expansion of the expandable particles. It is preferable that the adjustment is performed.
  • the non-intumescent base material layer (Y2) is provided on the surface of the expandable base material layer (Y1) opposite to the first pressure-sensitive adhesive layer (X1).
  • the second pressure-sensitive adhesive layer (X2) is laminated on the surface of the non-expandable base material layer (Y2).
  • the non-expandable base layer (Y2) absorbs.
  • the formation of irregularities on the adhesive surface of the second pressure-sensitive adhesive layer (X2) laminated on the non-expandable base material layer (Y2) is suppressed, and the cured sealed body is laminated on the adhesive surface. can do.
  • the first non-expandable so that irregularities are formed on the pressure-sensitive adhesive surface of the first pressure-sensitive adhesive layer (X1). It is preferable to adjust the storage elastic modulus E ′ of the base material layer (Y2-1) to be low. On the other hand, when the expandable particles expand, the second non-thermally expandable base material layer (Y2-2) is prevented from forming irregularities on the pressure-sensitive adhesive surface of the second pressure-sensitive adhesive layer (X2).
  • the storage elastic modulus E ′ is preferably adjusted to be high.
  • the storage elastic modulus E ′ of the first non-expandable base layer (Y2-1) when the expandable particles expand is equal to the second non-thermally expandable base layer (Y2) when the expandable particles expand.
  • -2) is preferably adjusted to be lower than the storage elastic modulus E ′.
  • a sealing object is placed on the pressure-sensitive adhesive surface of the expandable pressure-sensitive adhesive layer and cured.
  • the expansible adhesive layer which has mounted the sealing target object contains expansible particle
  • the expandable pressure-sensitive adhesive layer is a hard support.
  • a method of obtaining a cured sealing body by placing an object to be sealed on the non-intumescent pressure-sensitive adhesive layer is also conceivable.
  • the adhesive force of the expandable pressure-sensitive adhesive layer tends to be insufficient, and the sealing object is not sufficiently fixed to the hard support, the sealing object placed on the non-expandable pressure-sensitive adhesive layer
  • the pressure-sensitive adhesive is applied to the surface of the hard support when the double-sided pressure-sensitive adhesive sheet is peeled from the hard support by expanding the expandable particles. A part of the layer may remain, and it is necessary to perform a cleaning process of the support, which causes a decrease in productivity.
  • the expandable pressure-sensitive adhesive layer after expansion of the expandable particles is very brittle.
  • the expandable pressure-sensitive adhesive layer is located in the outermost layer. Part of the agent layer is likely to fall off or the expandable pressure-sensitive adhesive layer is easily peeled off.
  • the dropped expandable pressure-sensitive adhesive layer adheres to various devices in the production environment and contaminates the device, the device needs to be cleaned, which causes a decrease in productivity.
  • the pressure-sensitive adhesive sheet used in the production method of the present invention has a base material (Y) including at least an inflatable base material layer (Y1) containing inflatable particles and a non-inflatable base material layer (Y2), and is inflated.
  • a base material including at least an inflatable base material layer (Y1) containing inflatable particles and a non-inflatable base material layer (Y2), and is inflated.
  • the adhesive particles expand, the adhesive surface of the first pressure-sensitive adhesive layer (X1) is adjusted so that irregularities are formed. Therefore, the freedom degree of selection of the adhesive composition which is a forming material of the 1st adhesive layer (X1) and the 2nd adhesive layer (X2) is also high.
  • the first pressure-sensitive adhesive layer (X1) and the second pressure-sensitive adhesive are not considered without considering the expandability of the expandable particles. It is possible to select the adhesive resin used for the agent layer (X2).
  • the first pressure-sensitive adhesive layer (X1) to be attached to the hard support is a non-expandable pressure-sensitive adhesive layer and does not need to contain expandable particles, and therefore can be sufficiently fixed to the hard support. In addition, it is possible to effectively suppress adverse effects such as misalignment of the sealing object and adhesion of the sealing resin to the exposed surface of the sealing object due to insufficient fixation between the sealing object and the hard support.
  • the expandable base material layer (Y1) containing the expanded particles after expansion is not located at least in the outermost layer, and the pressure-sensitive adhesive layer It has a certain degree of strength as compared with the case where it contains expansive particles. Therefore, dropping off of the expandable base material layer (Y1) after the expansion is difficult to occur.
  • the first pressure-sensitive adhesive layer (X1) located in the outermost layer is a non-expandable pressure-sensitive adhesive layer and does not need to contain expandable particles. Defects such as dropping of one adhesive layer (X1) are unlikely to occur. Therefore, in the manufacturing method of the present invention, since contamination within the manufacturing environment can be effectively suppressed, there is no need for a cleaning step accompanying the contamination, and excellent productivity can be exhibited.
  • the pressure-sensitive adhesive sheet used in one embodiment of the present invention has irregularities on the pressure-sensitive adhesive surface of the first pressure-sensitive adhesive layer (X1) attached to the hard support due to the expansion of the expandable particles, and the hard support and the first pressure-sensitive adhesive. At the interface P with the layer (X1), separation can be easily performed at a time with a slight force.
  • the peeling force (F 1 ) when the expandable particles are expanded and separated at the interface P is usually 0 to 2000 mN / 25 mm, preferably 0 to 1000 mN / It is 25 mm, more preferably 0 to 150 mN / 25 mm, still more preferably 0 to 100 mN / 25 mm, and still more preferably 0 to 50 mN / 25 mm.
  • the peel force (F 1) is in the case of 0 mN / 25 mm, even trying to measure the peel strength by the method described in Example, includes the case where the measurement impossible because peel strength is too small.
  • the first adhesive layer (X1) has a higher adhesive force.
  • the peeling force (F 0 ) when separating at the interface P before the expansion of the expandable particles is preferably 0.05 to 10.0 N / 25 mm.
  • the release force (F 0) can also be regarded as the adhesive strength of the first adhesive layer to the rigid support member (X1).
  • the ratio [(F 1 ) / (F 0 )] between the peel force (F 1 ) and the peel force (F 0 ) is preferably 0 to 0.9, more preferably Is 0 to 0.8, more preferably 0 to 0.5, and still more preferably 0 to 0.2.
  • the release force (F 1) is a value measured under the environment when the expandable particles are expanded.
  • the temperature condition for measuring the peel force (F 1 ) may be equal to or higher than the expansion start temperature (t) of the thermally expandable particles.
  • the temperature condition for measuring the peeling force (F 0 ) may be any temperature at which the expandable particles do not expand, and is basically room temperature (23 ° C.).
  • more specific measurement conditions and measurement methods for the peel force (F 1 ) and the peel force (F 0 ) are based on the methods described in the examples.
  • the adhesive strength of the second pressure-sensitive adhesive layer (X2) at room temperature (23 ° C.) is preferably 0.1 to 10.0 N / 25 mm, more preferably 0. The range is from 0.2 to 8.0 N / 25 mm, more preferably from 0.4 to 6.0 N / 25 mm, and still more preferably from 0.5 to 4.0 N / 25 mm.
  • the adhesive strength of the second pressure-sensitive adhesive layer (X2) means a value measured by the method described in Examples.
  • each layer which comprises the adhesive sheet used by 1 aspect of this invention is demonstrated.
  • the base material (Y) included in the pressure-sensitive adhesive sheet used in one embodiment of the present invention includes at least an expandable base material layer (Y1) containing inflatable particles and a non-expandable base material layer (Y2).
  • a base material (Y) like the adhesive sheet 1a shown to Fig.1 (a), an expandable base material layer (Y1) and a non-expandable base material layer (Y2) are each laminated
  • the first non-thermally expandable base layer (Y2-1) and the second non-expandable base layer (Y2-1) are formed on both sides of the expandable base layer (Y1).
  • a configuration in which a non-thermally expandable base material layer (Y2-2) is provided may be employed.
  • the base material (Y) included in the pressure-sensitive adhesive sheet used in one embodiment of the present invention has a configuration in which an adhesive layer is provided between the inflatable base material layer (Y1) and the non-inflatable base material layer (Y2). May be.
  • An adhesive layer may be provided between the conductive base material layer (Y2-2).
  • the adhesive layer can be formed from a general adhesive or a pressure-sensitive adhesive composition that is a material for forming the first pressure-sensitive adhesive layer (X1) and the second pressure-sensitive adhesive layer (X2).
  • the expansion of the expandable particles causes unevenness on the adhesive surface of the first pressure-sensitive adhesive layer (X1), while suppressing the formation of unevenness on the adhesive surface of the second pressure-sensitive adhesive layer (X2).
  • the base material (Y) is provided with at least an inflatable base material layer (Y1) and a non-expandable base material layer (Y2) on the outermost surface.
  • the base material (Y) formed by laminating is mentioned.
  • the expandable substrate layer (Y1) and the non-expandable substrate layer (Y2) constituting the substrate (Y) are both non-adhesive layers.
  • the determination as to whether or not the layer is a non-adhesive layer is made if the probe tack value measured in accordance with JIS Z0237: 1991 is less than 50 mN / 5 mm ⁇ with respect to the surface of the target layer. Is judged as a “non-sticky layer”.
  • the probe tack values on the surfaces of the expandable base material layer (Y1) and the non-expandable base material layer (Y2) of the pressure-sensitive adhesive sheet (I) used in one embodiment of the present invention are each independently usually less than 50 mN / 5 mm ⁇ .
  • the specific measuring method of the probe tack value on the surface of a thermally expansible base material is based on the method as described in an Example.
  • the thickness of the substrate (Y) is preferably 15 to 2000 ⁇ m, more preferably 25 to 1500 ⁇ m, still more preferably 30 to 1000 ⁇ m, and still more preferably 40 to 500 ⁇ m. is there.
  • the thickness of the expandable substrate (Y1) before expansion of the expandable particles is preferably 10 to 1000 ⁇ m, more preferably 20 to 700 ⁇ m, still more preferably 25 to 500 ⁇ m, and still more preferably 30 to 300 ⁇ m.
  • the thickness of the non-expandable substrate (Y2) is preferably 10 to 1000 ⁇ m, more preferably 20 to 700 ⁇ m, still more preferably 25 to 500 ⁇ m, and still more preferably 30 to 300 ⁇ m.
  • a plurality of expandable substrates (Y1) or non-expandable substrates (Y2) exist via other layers as in the adhesive sheet 1b shown in FIG. 1 (b).
  • the thickness of said expansible base material (Y1) or a non-expandable base material (Y2) means the thickness per each layer.
  • the thickness ratio between the expandable base material layer (Y1) and the non-thermally expandable base material layer (Y2) before expansion of the expandable particles [(Y1) / ( Y2)] is preferably 0.02 to 200, more preferably 0.03 to 150, and still more preferably 0.05 to 100.
  • the thickness ratio [(Y1) / (X1)] is preferably 0.2 or more, more preferably 0.5 or more, still more preferably 1.0 or more, and still more preferably 5.0 or more. Also, it is preferably 1000 or less, more preferably 200 or less, still more preferably 60 or less, and still more preferably 30 or less.
  • the ratio [(Y2) / (X2)] is preferably 0.1 or more, more preferably 0.2 or more, still more preferably 0.3 or more, and preferably 20 or less, more preferably 10 or less. More preferably, it is 5 or less.
  • the expandable substrate layer (Y1) and the non-expandable substrate layer (Y2) constituting the substrate (Y) will be described.
  • the expandable substrate layer (Y1) constituting the substrate (Y) is a layer that contains expandable particles and can be expanded by a predetermined expansion treatment.
  • the content of the expandable particles in the expandable substrate layer (Y1) is preferably 1 to 40% by mass, more preferably 5%, based on the total mass (100% by mass) of the expandable substrate layer (Y1). It is ⁇ 35% by mass, more preferably 10 to 30% by mass, and still more preferably 15 to 25% by mass.
  • the surface of the expandable base material layer (Y1) is a surface formed by an oxidation method, a roughening method, or the like.
  • Treatment, easy adhesion treatment, or primer treatment may be performed.
  • the oxidation method include corona discharge treatment, plasma discharge treatment, chromic acid treatment (wet), hot air treatment, ozone, and ultraviolet irradiation treatment.
  • the unevenness method include sand blast method and solvent treatment method. Etc.
  • the expandable particles contained in the expandable substrate layer (Y1) may be any particles that expand by performing a predetermined treatment, such as thermally expandable particles that expand by heating at a predetermined temperature or higher, Examples include UV-expandable particles that absorb a predetermined amount of ultraviolet rays to generate gas and expand inside the particles.
  • the volume expansion coefficient of the expandable particles is preferably 1.5 to 100 times, more preferably 2 to 80 times, still more preferably 2.5 to 60 times, and still more preferably 3 to 40 times.
  • the average particle diameter of the expandable particles before expansion at 23 ° C. is preferably 3 to 100 ⁇ m, more preferably 4 to 70 ⁇ m, still more preferably 6 to 60 ⁇ m, and still more preferably 10 to 50 ⁇ m.
  • the average particle size of the expandable particles is the volume-median particle size (D 50 ) and is measured using a laser diffraction particle size distribution measuring device (for example, product name “Mastersizer 3000” manufactured by Malvern). In the particle distribution of the expanded particles, it means a particle size corresponding to 50% of the cumulative volume frequency calculated from the smaller particle size of the expandable particles.
  • the 90% particle diameter (D 90 ) of the expandable particles before expansion at 23 ° C. is preferably 10 to 150 ⁇ m, more preferably 20 to 100 ⁇ m, still more preferably 25 to 90 ⁇ m, and still more preferably 30 to 80 ⁇ m. .
  • the 90% particle size (D 90 ) of the expandable particles is the particle distribution of the expandable particles measured using a laser diffraction particle size distribution measuring device (for example, product name “Mastersizer 3000” manufactured by Malvern). In FIG. 5, the particle size corresponding to 90% of the cumulative volume frequency calculated from the smaller particle size of the expandable particles.
  • the expandable particles are preferably thermally expandable particles having an expansion start temperature (t) of 60 to 270 ° C. That is, the expandable substrate layer (Y1) is preferably a thermally expandable substrate layer (Y1-1) containing thermally expandable particles having an expansion start temperature (t) of 60 to 270 ° C.
  • the conductive base material layer (Y1-1) more preferably satisfies the following requirement (1).
  • the storage elastic modulus E ′ (t) of the thermally expandable substrate layer (Y1-1) at the expansion start temperature (t) of the thermally expandable particles is 1.0 ⁇ 10 7 Pa It is as follows. In the present specification, the storage elastic modulus E ′ of the thermally expandable base material layer (Y1-1) at a predetermined temperature means a value measured by the method described in the examples.
  • the requirement (1) can be said to be an index indicating the rigidity of the thermally expandable substrate layer (Y1-1) immediately before the thermally expandable particles expand. That is, when the thermally expandable particles expand, if the thermally expandable substrate layer (Y1-1) is flexible enough to satisfy the above requirement (1), the thermally expandable substrate layer (Y1 As a result, unevenness is likely to be formed on the surface of -1), and unevenness is also likely to occur on the adhesive surface of the first pressure-sensitive adhesive layer (X1). As a result, it is possible to easily separate them with a slight force at the interface P between the hard support and the first pressure-sensitive adhesive layer (X1).
  • the storage elastic modulus E ′ (t) defined by requirement (1) of the thermally expandable base material layer (Y1-1) is preferably 9.0 ⁇ 10 6 Pa or less, more preferably 8.0. ⁇ 10 6 Pa or less, more preferably 6.0 ⁇ 10 6 Pa or less, and even more preferably 4.0 ⁇ 10 6 Pa or less.
  • the flow of the expanded heat-expandable particles is suppressed, the shape maintaining property of the unevenness generated on the surface of the heat-expandable base material layer (Y1-1) is improved, and the pressure-sensitive adhesive surface of the first pressure-sensitive adhesive layer (X1) is improved.
  • the storage elastic modulus E ′ (t) defined by the requirement (1) of the thermally expandable base material layer (Y1-1) is preferably 1.0 ⁇ 10 3 Pa or more. Preferably it is 1.0 ⁇ 10 4 Pa or more, more preferably 1.0 ⁇ 10 5 Pa or more.
  • the thermally expandable base material layer (Y1-1) preferably satisfies the following requirement (2), and more preferably satisfies the requirement (2) together with the requirement (1).
  • the storage elastic modulus E ′ (23) of the thermally expandable base material layer (Y1-1) at 23 ° C. is 1.0 ⁇ 10 6 Pa or more.
  • thermally expandable base material layer (Y1-1) that satisfies the above requirement (2), it is possible to prevent displacement when the sealing object is placed on the adhesive surface of the second adhesive layer (X2). In addition, excessive sinking of the sealing object into the second pressure-sensitive adhesive layer (X2) can also be prevented.
  • the storage elastic modulus E ′ (23) of the thermally expandable base material layer (Y1-1) defined by the above requirement (2) is preferably 5.0 ⁇ 10 6 to 5.0 ⁇ 10 12 Pa. More preferably 1.0 ⁇ 10 7 to 1.0 ⁇ 10 12 Pa, still more preferably 5.0 ⁇ 10 7 to 1.0 ⁇ 10 11 Pa, and still more preferably 1.0 ⁇ 10 8 to 1. 0 ⁇ 10 10 Pa.
  • the heat-expandable particles contained in the heat-expandable base material layer (Y1-1) are preferably heat-expandable particles having an expansion start temperature (t) of 60 to 270 ° C.
  • the expansion start temperature (t) of the thermally expandable particles means a value measured based on the following method.
  • Measurement method of expansion start temperature (t) of thermally expandable particles To an aluminum cup having a diameter of 6.0 mm (inner diameter: 5.65 mm) and a depth of 4.8 mm, 0.5 mg of thermally expandable particles to be measured is added, and an aluminum lid (diameter of 5.6 mm, thickness of 0.2 mm) is added from above. 1 mm) is prepared.
  • the height of the sample is measured from the upper part of the aluminum lid to the sample with a force of 0.01 N applied by a pressurizer. Then, with a force of 0.01 N applied by the pressurizer, heating is performed from 20 ° C. to 300 ° C. at a rate of temperature increase of 10 ° C./min, and the amount of displacement of the pressurizer in the vertical direction is measured.
  • the displacement start temperature be the expansion start temperature (t).
  • the thermally expandable particles are microencapsulated foaming agents composed of an outer shell composed of a thermoplastic resin and an encapsulated component encapsulated in the outer shell and vaporized when heated to a predetermined temperature.
  • a thermoplastic resin constituting the outer shell of the microencapsulated foaming agent include vinylidene chloride-acrylonitrile copolymer, polyvinyl alcohol, polyvinyl butyral, polymethyl methacrylate, polyacrylonitrile, polyvinylidene chloride, and polysulfone.
  • Examples of the inclusion component contained in the outer shell include propane, butane, pentane, hexane, heptane, octane, nonane, decane, isobutane, isopentane, isohexane, isoheptane, isooctane, isononane, isodecane, cyclopropane, cyclobutane, cyclopentane.
  • the expandable substrate layer (Y1) is preferably formed from a resin composition (y) containing a resin and expandable particles.
  • the substrate additive include an ultraviolet absorber, a light stabilizer, an antioxidant, an antistatic agent, a slip agent, an antiblocking agent, and a colorant.
  • These base material additives may be used alone or in combination of two or more. When these base material additives are contained, the content of each base material additive is preferably 0.0001 to 20 parts by mass, more preferably 0.001 to about 100 parts by mass of the resin. 10 parts by mass.
  • the expandable particles contained in the resin composition (y), which is a material for forming the expandable substrate layer (Y1), are as described above, and are preferably thermally expandable particles.
  • the content of the expandable particles is preferably 1 to 40% by mass, more preferably 5 to 35% by mass, and further preferably 10 to 10% by mass with respect to the total amount (100% by mass) of the active ingredients of the resin composition (y). It is 30% by mass, more preferably 15 to 25% by mass.
  • the resin contained in the resin composition (y) that is a material for forming the expandable base material layer (Y1) may be a non-adhesive resin or an adhesive resin. That is, even if the resin contained in the resin composition (y) is an adhesive resin, in the process of forming the expandable substrate layer (Y1) from the resin composition (y), the adhesive resin is a polymerizable compound. And the resulting resin becomes a non-adhesive resin, and the expandable base material layer (Y1) containing the resin may be non-adhesive.
  • the mass average molecular weight (Mw) of the resin contained in the resin composition (y) is preferably 1,000 to 1,000,000, more preferably 1,000 to 700,000, and still more preferably 1,000 to 500,000. Further, when the resin is a copolymer having two or more kinds of structural units, the form of the copolymer is not particularly limited, and any of a block copolymer, a random copolymer, and a graft copolymer It may be.
  • the content of the resin is preferably 50 to 99% by mass, more preferably 60 to 95% by mass, and still more preferably 65 to 90% by mass with respect to the total amount (100% by mass) of the active ingredients of the resin composition (y). %, More preferably 70 to 85% by mass.
  • the resin contained in the resin composition (y) is an acrylic urethane from the viewpoint of forming an expandable base layer (Y1) that easily forms irregularities on the surface when the expandable particles are expanded. It is preferable that 1 or more types chosen from a system resin and an olefin resin are included. Moreover, as said acrylic urethane type resin, the following resin (U1) is preferable.
  • An acrylic urethane resin (U1) obtained by polymerizing a urethane prepolymer (UP) and a vinyl compound containing a (meth) acrylic acid ester.
  • urethane prepolymer (UP) serving as the main chain of the acrylic urethane resin (U1) include a reaction product of a polyol and a polyvalent isocyanate.
  • the urethane prepolymer (UP) is preferably obtained by further subjecting it to a chain extension reaction using a chain extender.
  • Examples of the polyol used as a raw material for the urethane prepolymer (UP) include alkylene type polyols, ether type polyols, ester type polyols, ester amide type polyols, ester / ether type polyols, and carbonate type polyols. These polyols may be used independently and may use 2 or more types together.
  • the polyol used in one embodiment of the present invention is preferably a diol, more preferably an ester diol, an alkylene diol, and a carbonate diol, and even more preferably an ester diol and a carbonate diol.
  • ester diol examples include alkane diols such as 1,3-propanediol, 1,4-butanediol, 1,5-pentanediol, neopentyl glycol, 1,6-hexanediol; ethylene glycol, propylene glycol, One or more selected from diols such as alkylene glycols such as diethylene glycol and dipropylene glycol; phthalic acid, isophthalic acid, terephthalic acid, naphthalenedicarboxylic acid, 4,4-diphenyldicarboxylic acid, diphenylmethane-4 , 4'-dicarboxylic acid, succinic acid, adipic acid, azelaic acid, sebacic acid, het acid, maleic acid, fumaric acid, itaconic acid, cyclohexane-1,3-dicarboxylic acid, cyclohexane-1,4-dicarboxyl
  • alkylene type diol examples include alkane diols such as 1,3-propanediol, 1,4-butanediol, 1,5-pentanediol, neopentyl glycol, 1,6-hexanediol; ethylene glycol, propylene glycol, And alkylene glycols such as diethylene glycol and dipropylene glycol; polyalkylene glycols such as polyethylene glycol, polypropylene glycol, and polybutylene glycol; polyoxyalkylene glycols such as polytetramethylene glycol; and the like.
  • alkane diols such as 1,3-propanediol, 1,4-butanediol, 1,5-pentanediol, neopentyl glycol, 1,6-hexanediol
  • ethylene glycol, propylene glycol And alkylene glycols such as diethylene glycol and dipropylene glycol
  • Examples of the carbonate type diol include 1,4-tetramethylene carbonate diol, 1,5-pentamethylene carbonate diol, 1,6-hexamethylene carbonate diol, 1,2-propylene carbonate diol, and 1,3-propylene carbonate diol. 2,2-dimethylpropylene carbonate diol, 1,7-heptamethylene carbonate diol, 1,8-octamethylene carbonate diol, 1,4-cyclohexane carbonate diol, and the like.
  • polyvalent isocyanate used as a raw material for the urethane prepolymer (UP) examples include aromatic polyisocyanates, aliphatic polyisocyanates, and alicyclic polyisocyanates. These polyvalent isocyanates may be used alone or in combination of two or more. These polyisocyanates may be a trimethylolpropane adduct-type modified product, a burette-type modified product reacted with water, or an isocyanurate-type modified product containing an isocyanurate ring.
  • the polyisocyanate used in one embodiment of the present invention is preferably diisocyanate, and 4,4′-diphenylmethane diisocyanate (MDI), 2,4-tolylene diisocyanate (2,4-TDI), 2,6 More preferred is at least one selected from tolylene diisocyanate (2,6-TDI), hexamethylene diisocyanate (HMDI), and alicyclic diisocyanate.
  • MDI 4,4′-diphenylmethane diisocyanate
  • 2,4-TDI 2,4-tolylene diisocyanate
  • 2,6 More preferred is at least one selected from tolylene diisocyanate (2,6-TDI), hexamethylene diisocyanate (HMDI), and alicyclic diisocyanate.
  • alicyclic diisocyanate examples include 3-isocyanate methyl-3,5,5-trimethylcyclohexyl isocyanate (isophorone diisocyanate, IPDI), 1,3-cyclopentane diisocyanate, 1,3-cyclohexane diisocyanate, 1,4-cyclohexane.
  • IPDI isophorone diisocyanate
  • Examples include diisocyanate, methyl-2,4-cyclohexane diisocyanate, methyl-2,6-cyclohexane diisocyanate, and isophorone diisocyanate (IPDI) is preferred.
  • the urethane prepolymer (UP) serving as the main chain of the acrylic urethane resin (U1) is a reaction product of a diol and a diisocyanate, and is a straight chain having ethylenically unsaturated groups at both ends.
  • a urethane prepolymer is preferred.
  • an NCO group at the end of the linear urethane prepolymer obtained by reacting a diol and a diisocyanate compound, and a hydroxyalkyl (meth) acrylate And a method of reacting with.
  • hydroxyalkyl (meth) acrylate examples include 2-hydroxyethyl (meth) acrylate, 2-hydroxypropyl (meth) acrylate, 3-hydroxypropyl (meth) acrylate, 2-hydroxybutyl (meth) acrylate, and 3-hydroxy Examples thereof include butyl (meth) acrylate and 4-hydroxybutyl (meth) acrylate.
  • the (meth) acrylic acid ester is preferably at least one selected from alkyl (meth) acrylates and hydroxyalkyl (meth) acrylates, and more preferably used in combination with alkyl (meth) acrylates and hydroxyalkyl (meth) acrylates.
  • the proportion of hydroxyalkyl (meth) acrylate to 100 parts by mass of alkyl (meth) acrylate is preferably 0.1 to 100 parts by mass, The amount is preferably 0.5 to 30 parts by mass, more preferably 1.0 to 20 parts by mass, and still more preferably 1.5 to 10 parts by mass.
  • the carbon number of the alkyl group of the alkyl (meth) acrylate is preferably 1 to 24, more preferably 1 to 12, still more preferably 1 to 8, and still more preferably 1 to 3.
  • hydroxyalkyl (meth) acrylate the same thing as the hydroxyalkyl (meth) acrylate used in order to introduce
  • vinyl compounds other than (meth) acrylic acid esters include aromatic hydrocarbon vinyl compounds such as styrene, ⁇ -methylstyrene, and vinyl toluene; vinyl ethers such as methyl vinyl ether and ethyl vinyl ether; vinyl acetate and vinyl propionate.
  • Polar group-containing monomers such as (meth) acrylonitrile, N-vinylpyrrolidone, (meth) acrylic acid, maleic acid, fumaric acid, itaconic acid, and meta (acrylamide). These may be used alone or in combination of two or more.
  • the content of the (meth) acrylic acid ester in the vinyl compound is preferably 40 to 100% by mass, more preferably 65 to 100% by mass, and still more preferably based on the total amount (100% by mass) of the vinyl compound. It is 80 to 100% by mass, more preferably 90 to 100% by mass.
  • the total content of alkyl (meth) acrylate and hydroxyalkyl (meth) acrylate in the vinyl compound is preferably 40 to 100% by mass, more preferably 65 to 100% by mass with respect to the total amount (100% by mass) of the vinyl compound.
  • the amount is 100% by mass, more preferably 80 to 100% by mass, and still more preferably 90 to 100% by mass.
  • the content ratio of the structural unit (u11) derived from the urethane prepolymer (UP) and the structural unit (u12) derived from the vinyl compound [(u11 ) / (U12)] is preferably 10/90 to 80/20, more preferably 20/80 to 70/30, still more preferably 30/70 to 60/40, and still more preferably 35 by mass ratio. / 65 to 55/45.
  • olefin resin examples include a polymer having at least a structural unit derived from an olefin monomer.
  • the olefin monomer is preferably an ⁇ -olefin having 2 to 8 carbon atoms, and specifically includes ethylene, propylene, butylene, isobutylene, 1-hexene and the like. Among these, ethylene and propylene are preferable.
  • olefinic resins for example, ultra low density polyethylene (VLDPE, density: 880 kg / m 3 or more 910 kg / m less than 3), low density polyethylene (LDPE, density: 910 kg / m 3 or more 915 kg / m less than 3 ), Medium density polyethylene (MDPE, density: 915 kg / m 3 or more and less than 942 kg / m 3 ), high density polyethylene (HDPE, density: 942 kg / m 3 or more), linear low density polyethylene, etc .; polypropylene resin (PP); polybutene resin (PB); ethylene-propylene copolymer; olefin elastomer (TPO); ethylene-vinyl acetate copolymer (EVA); ethylene-propylene- (5-ethylidene-2-norbornene), etc. Olefin terpolymers; and the like.
  • VLDPE ultra low density polyethylene
  • LDPE low density poly
  • the olefin resin may be a modified olefin resin further modified by one or more selected from acid modification, hydroxyl group modification, and acrylic modification.
  • an acid-modified olefin resin obtained by subjecting an olefin resin to acid modification a modified polymer obtained by graft polymerization of the above-mentioned unmodified olefin resin with an unsaturated carboxylic acid or its anhydride.
  • unsaturated carboxylic acid or its anhydride include maleic acid, fumaric acid, itaconic acid, citraconic acid, glutaconic acid, tetrahydrophthalic acid, aconitic acid, (meth) acrylic acid, maleic anhydride, itaconic anhydride.
  • Glutaconic anhydride citraconic anhydride, aconitic anhydride, norbornene dicarboxylic anhydride, tetrahydrophthalic anhydride, and the like.
  • unsaturated carboxylic acid or its anhydride may be used independently, and may use 2 or more types together.
  • an acrylic modified olefin resin obtained by subjecting an olefin resin to acrylic modification a modification obtained by graft polymerization of an alkyl (meth) acrylate as a side chain to the above-mentioned unmodified olefin resin as a main chain.
  • a polymer is mentioned.
  • the number of carbon atoms of the alkyl group contained in the alkyl (meth) acrylate is preferably 1-20, more preferably 1-16, and still more preferably 1-12.
  • said alkyl (meth) acrylate the same thing as the compound which can be selected as a below-mentioned monomer (a1 ') is mentioned, for example.
  • Examples of the hydroxyl group-modified olefin resin obtained by modifying the olefin resin with a hydroxyl group include a modified polymer obtained by graft-polymerizing a hydroxyl group-containing compound to the above-mentioned unmodified olefin resin as the main chain.
  • Examples of the hydroxyl group-containing compound include 2-hydroxyethyl (meth) acrylate, 2-hydroxypropyl (meth) acrylate, 3-hydroxypropyl (meth) acrylate, 2-hydroxybutyl (meth) acrylate, and 3-hydroxybutyl.
  • Examples include hydroxyalkyl (meth) acrylates such as (meth) acrylate and 4-hydroxybutyl (meth) acrylate; unsaturated alcohols such as vinyl alcohol and allyl alcohol.
  • the resin composition (y) may contain a resin other than the acrylic urethane-based resin and the olefin-based resin as long as the effects of the present invention are not impaired.
  • resins include vinyl resins such as polyvinyl chloride, polyvinylidene chloride, polyvinyl alcohol, ethylene-vinyl acetate copolymer, ethylene-vinyl alcohol copolymer; polyethylene terephthalate, polybutylene terephthalate, polyethylene naphthalate.
  • Polyester resin such as phthalate; polystyrene; acrylonitrile-butadiene-styrene copolymer; cellulose triacetate; polycarbonate; polyurethane not applicable to acrylic urethane resin; polymethylpentene; polysulfone; polyetheretherketone; polyethersulfone; Sulfides; Polyimide resins such as polyetherimide and polyimide; Polyamide resins; Acrylic resins; Fluorine resins and the like.
  • the resin composition (y) contains a resin other than the acrylic urethane resin and the olefin resin. A smaller ratio is preferable.
  • the content ratio of the resin other than the acrylic urethane-based resin and the olefin-based resin is preferably less than 30 parts by weight, more preferably 20 parts by weight with respect to 100 parts by weight of the total amount of the resin contained in the resin composition (y). Less than, more preferably less than 10 parts by weight, still more preferably less than 5 parts by weight, and even more preferably less than 1 part by weight.
  • solvent-free resin composition (y1) As an aspect of the resin composition (y), a solvent comprising an oligomer having an ethylenically unsaturated group having a mass average molecular weight (Mw) of 50000 or less, an energy ray polymerizable monomer, and the above-mentioned expandable particles, And a solvent-free resin composition (y1) that does not contain the above.
  • Mw mass average molecular weight
  • a solvent-free resin composition (y1) that does not contain the above.
  • the solventless resin composition (y1) no solvent is blended, but the energy beam polymerizable monomer contributes to the improvement of the plasticity of the oligomer.
  • an inflatable substrate layer (Y1) that easily forms irregularities on the surface when the expandable particles expand is formed.
  • the type, shape, and blending amount (content) of the expandable particles blended in the solventless resin composition (y1) are the same as those of the resin composition (y) and are as described above.
  • the mass average molecular weight (Mw) of the oligomer contained in the solventless resin composition (y1) is 50000 or less, preferably 1000 to 50000, more preferably 2000 to 40000, and still more preferably 3000 to 35000. More preferably, it is 4000-30000.
  • oligomer As said oligomer, what is necessary is just to have an ethylenically unsaturated group whose mass mean molecular weight is 50000 or less among resin contained in the above-mentioned resin composition (y), but the above-mentioned urethane prepolymer (UP Is preferred.
  • UP Is preferred As the oligomer, a modified olefin resin having an ethylenically unsaturated group can also be used.
  • the total content of the oligomer and the energy beam polymerizable monomer in the solventless resin composition (y1) is preferably from 50 to the total amount (100% by mass) of the solventless resin composition (y1). It is 99% by mass, more preferably 60 to 95% by mass, still more preferably 65 to 90% by mass, and still more preferably 70 to 85% by mass.
  • Examples of the energy ray polymerizable monomer include isobornyl (meth) acrylate, dicyclopentenyl (meth) acrylate, dicyclopentanyl (meth) acrylate, dicyclopentenyloxy (meth) acrylate, cyclohexyl (meth) acrylate, adamantane ( Alicyclic polymerizable compounds such as (meth) acrylate and tricyclodecane acrylate; Aromatic polymerizable compounds such as phenylhydroxypropyl acrylate, benzyl acrylate and phenol ethylene oxide modified acrylate; Tetrahydrofurfuryl (meth) acrylate, morpholine acrylate, N- And heterocyclic polymerizable compounds such as vinylpyrrolidone and N-vinylcaprolactam. These energy beam polymerizable monomers may be used independently and may use 2 or more types together.
  • the blending ratio of the oligomer and the energy beam polymerizable monomer is preferably 20/80 to 90/10, more preferably 30/70 to 85/15, still more preferably 35/65. ⁇ 80/20.
  • the solventless resin composition (y1) further comprises a photopolymerization initiator.
  • the curing reaction can be sufficiently advanced even by irradiation with energy rays having relatively low energy.
  • photopolymerization initiator examples include 1-hydroxy-cyclohexyl-phenyl-ketone, benzoin, benzoin methyl ether, benzoin ethyl ether, benzoin propyl ether, benzyl phenyl sulfide, tetramethylthiuram monosulfide, azobisisobutyrol. Nitrile, dibenzyl, diacetyl, 8-chloranthraquinone and the like can be mentioned. These photoinitiators may be used independently and may use 2 or more types together.
  • the blending amount of the photopolymerization initiator is preferably 0.01 to 5 parts by mass, more preferably 0.01 to 4 parts by mass with respect to the total amount (100 parts by mass) of the oligomer and the energy ray polymerizable monomer.
  • the amount is preferably 0.02 to 3 parts by mass.
  • Non-expandable base material layer (Y2) Examples of the material for forming the non-intumescent base material layer (Y2) constituting the base material (Y) include paper materials, resins, metals, and the like. Examples of the paper material include thin paper, medium quality paper, high quality paper, impregnated paper, coated paper, art paper, sulfuric acid paper, glassine paper, and the like.
  • the resin examples include polyolefin resins such as polyethylene and polypropylene; vinyl resins such as polyvinyl chloride, polyvinylidene chloride, polyvinyl alcohol, ethylene-vinyl acetate copolymer, and ethylene-vinyl alcohol copolymer; polyethylene terephthalate, poly Polyester resins such as butylene terephthalate and polyethylene naphthalate; polystyrene; acrylonitrile-butadiene-styrene copolymer; cellulose triacetate; polycarbonate; urethane resin such as polyurethane and acrylic-modified polyurethane; polymethylpentene; polysulfone; polyether ether ketone; Polyethersulfone; Polyphenylene sulfide; Polyimide resin such as polyetherimide and polyimide; Polyamide resin; Acrylic resin; Tsu Motokei resin, and the like.
  • the metal examples include aluminum, tin, chromium, and
  • These forming materials may be composed of one kind or in combination of two or more kinds.
  • a non-intumescent base material layer (Y2) using two or more kinds of forming materials in combination a paper film is laminated with a thermoplastic resin such as polyethylene, or a metal film is formed on the surface of a resin film or sheet containing a resin. And the like.
  • a method for forming the metal layer for example, a method of depositing the metal by a PVD method such as vacuum deposition, sputtering, or ion plating, or a metal foil made of the metal is attached using a general adhesive. And the like.
  • the non-expandable base layer (Y2) contains a resin
  • the non-intumescent base material layer (Y2) contains a resin
  • it may contain the above-mentioned base material additive that can be contained in the resin composition (y) together with the resin.
  • the non-intumescent substrate layer (Y2) is present at a position farther from the first pressure-sensitive adhesive layer (X1) than the above-described inflatable substrate layer (Y1), and the inflatable substrate layer (Y1) ) And the first pressure-sensitive adhesive layer (X1), there is no non-expandable base layer (Y2), and the non-expandable base layer (Y2) when the expandable particles expand.
  • the storage elastic modulus E ′ is preferably larger than the storage elastic modulus E ′ of the expandable base material layer (Y1) when the expandable particles expand.
  • the expandable base material layer is expanded by the expansion of the expandable particles.
  • the unevenness generated on the surface of (Y1) is transmitted to the first pressure-sensitive adhesive layer (X1) without interposing the non-intumescent base material layer (Y2), and on the pressure-sensitive adhesive surface of the first pressure-sensitive adhesive layer (X1).
  • unevenness is likely to occur.
  • the storage elastic modulus E ′ of the non-expandable base material layer (Y2) is larger than the storage elastic modulus E ′ of the expandable base material layer (Y1).
  • the surface of the expandable substrate layer (Y1) on the non-expandable substrate layer (Y2) side is prevented from being uneven, and as a result, the first of the expandable substrate layer (Y1). Unevenness is likely to occur on the surface on the pressure-sensitive adhesive layer (X1) side, and therefore unevenness is also likely to occur on the adhesive surface of the first pressure-sensitive adhesive layer (X1).
  • the storage elastic modulus E ′ of the non-expandable base material layer (Y2) when the expandable particles are expanded is as described above from the viewpoint of easily forming irregularities on the adhesive surface of the first adhesive layer (X1).
  • the pressure is 1.0 MPa or more.
  • the storage elastic modulus E ′ of the non-expandable base material layer (Y2) when the expandable particles expand is preferably 1.0 to 5.0 ⁇ 10 2 MPa, more preferably 1.0.
  • the storage elastic modulus of the non-expandable base material layer (Y2) at 23 ° C. E ′ (23) is preferably 5.0 ⁇ 10 1 to 5.0 ⁇ 10 4 MPa, more preferably 1.0 ⁇ 10 2 to 1.0 ⁇ 10 4 MPa, and even more preferably 5.0 ⁇ 10. 2 to 5.0 ⁇ 10 3 MPa.
  • a non-expandable base material layer (Y2) is a non-expandable layer judged based on the above-mentioned method.
  • the volume change rate (%) of the non-expandable base material layer (Y2) calculated from the above formula is less than 5% by volume, preferably less than 2% by volume, more preferably less than 1% by volume. More preferably, it is less than 0.1 volume%, More preferably, it is less than 0.01 volume%.
  • a non-expandable base material layer (Y2) may contain a thermally expansible particle.
  • a resin contained in the non-expandable base material layer (Y2) it is possible to adjust the volume change rate to the above range even if thermally expandable particles are included.
  • the specific content of the heat-expandable particles is usually less than 3% by mass, preferably less than 1% by mass, and more preferably relative to the total mass (100% by mass) of the non-expandable base material layer (Y2). It is less than 0.1% by mass, more preferably less than 0.01% by mass, and still more preferably less than 0.001% by mass.
  • the pressure-sensitive adhesive sheet used in one embodiment of the present invention has a first pressure-sensitive adhesive layer (X1) and a second pressure-sensitive adhesive layer (X2), which are non-intumescent pressure-sensitive adhesive layers.
  • the pressure-sensitive adhesive surface of the first pressure-sensitive adhesive layer (X1) is affixed to a hard support, and a sealing object is placed on the pressure-sensitive adhesive surface of the second pressure-sensitive adhesive layer (X2). A cured encapsulant is formed.
  • first pressure-sensitive adhesive layer (X1) and the second pressure-sensitive adhesive layer (X2) are non-expandable pressure-sensitive adhesive layers, the position of the sealing target due to insufficient fixation between the sealing target and the hard support It is possible to effectively suppress adverse effects such as displacement and adhesion of the sealing resin to the exposed surface of the object to be sealed.
  • first pressure-sensitive adhesive layer (X1) is a non-intumescent pressure-sensitive adhesive layer, in addition to the above effects, in the cured sealed body with the pressure-sensitive adhesive sheet after separation from the cured support, The adhesive layer (X1) can be prevented from falling off and the like, which can contaminate various devices in the manufacturing environment.
  • the first pressure-sensitive adhesive layer (X1) has high adhesiveness with the hard support before expansion of the expandable particles contained in the expandable base material layer (Y1), and the sealing object is sufficient for the hard support.
  • the property which can be fixed to is required.
  • the storage shear modulus G ′ (23) of the first pressure-sensitive adhesive layer (X1) at 23 ° C. is preferably 1.0 ⁇ 10 8 Pa or less, more preferably 5.0 ⁇ 10 7 Pa or less. More preferably, it is 1.0 ⁇ 10 7 Pa or less.
  • the storage shear modulus G ′ (23) of the first pressure-sensitive adhesive layer (X1) at 23 ° C. is preferably 1.0 ⁇ 10 4 Pa or more, more preferably 5.0 ⁇ 10 4 Pa or more. More preferably, it is 1.0 ⁇ 10 5 Pa or more.
  • the second pressure-sensitive adhesive layer (X2) is required to have not only adhesion with the sealing object but also adhesion with a cured sealing body formed by sealing the sealing object with a sealing material.
  • the storage shear modulus G ′ (23) of the second pressure-sensitive adhesive layer (X2) at 23 ° C. is preferably 1.0 ⁇ 10 4 to 1.0 ⁇ 10 8 Pa, more preferably 5 It is 0.0 ⁇ 10 4 to 5.0 ⁇ 10 7 Pa, more preferably 9.0 ⁇ 10 4 to 1.0 ⁇ 10 7 Pa.
  • the storage shear elastic modulus G '(23) of the 1st adhesive layer (X1) and the 2nd adhesive layer (X2) means the value measured by the method as described in an Example. .
  • the thickness of the first pressure-sensitive adhesive layer (X1) is preferably 1 to 60 ⁇ m, more preferably 2 to 50 ⁇ m, still more preferably 3 to 40 ⁇ m, and still more preferably 5 to 30 ⁇ m.
  • the thickness of the second pressure-sensitive adhesive layer (X2) is preferably 1 to 60 ⁇ m, more preferably 2 to 50 ⁇ m, still more preferably 3 to 40 ⁇ m, and still more preferably 5 to 30 ⁇ m.
  • the first pressure-sensitive adhesive layer (X1) and the second pressure-sensitive adhesive layer (X2) can be formed from a pressure-sensitive adhesive composition (x) containing a pressure-sensitive adhesive resin.
  • adhesive composition (x) may contain additives for adhesives, such as a crosslinking agent, a tackifier, a polymeric compound, a polymerization initiator, as needed.
  • additives for adhesives such as a crosslinking agent, a tackifier, a polymeric compound, a polymerization initiator, as needed.
  • any polymer may be used as long as it has adhesiveness and has a mass average molecular weight (Mw) of 10,000 or more.
  • the mass average molecular weight (Mw) of the adhesive resin used in one embodiment of the present invention is preferably 10,000 to 2,000,000, more preferably 20,000 to 1,500,000, and still more preferably 30,000, from the viewpoint of improving adhesive force. ⁇ 1 million.
  • the adhesive resin examples include rubber resins such as acrylic resins, urethane resins, and polyisobutylene resins, polyester resins, olefin resins, silicone resins, and polyvinyl ether resins. These adhesive resins may be used alone or in combination of two or more. Further, when these adhesive resins are copolymers having two or more kinds of structural units, the form of the copolymer is not particularly limited, and a block copolymer, a random copolymer, and a graft copolymer are not limited. Any of polymers may be used.
  • the adhesive resin used in one embodiment of the present invention may be an energy ray curable adhesive resin in which a polymerizable functional group is introduced into the side chain of the above-mentioned adhesive resin.
  • the adhesive force can be reduced by irradiating energy rays. Therefore, the obtained cured sealing body can be easily separated from the second pressure-sensitive adhesive layer (X2).
  • the polymerizable functional group include a (meth) acryloyl group and a vinyl group.
  • energy rays include ultraviolet rays and electron beams, but ultraviolet rays are preferred.
  • the energy ray hardening-type adhesive composition containing the monomer or oligomer which has a polymerizable functional group may be sufficient.
  • These energy ray curable pressure-sensitive adhesive compositions preferably further contain a photopolymerization initiator.
  • a photopolymerization initiator By containing the photopolymerization initiator, the curing reaction can be sufficiently advanced even by irradiation with energy rays having relatively low energy.
  • a photoinitiator the same thing as what is mix
  • the content of the photopolymerization initiator is preferably 0.01 to 10 parts by mass, more preferably 100 parts by mass of the energy ray-curable adhesive resin or 100 parts by mass of the monomer or oligomer having a polymerizable functional group.
  • the amount is 0.03 to 5 parts by mass, more preferably 0.05 to 2 parts by mass.
  • the adhesive resin preferably contains an acrylic resin from the viewpoint of developing an excellent adhesive force.
  • the first pressure-sensitive adhesive layer (X1) by forming the first pressure-sensitive adhesive layer (X1) from a pressure-sensitive adhesive composition containing an acrylic resin, it is possible to easily form irregularities on the surface of the first pressure-sensitive adhesive layer.
  • the content of the acrylic resin in the adhesive resin is preferably 30 to 100% by mass, more preferably 50%, based on the total amount (100% by mass) of the adhesive resin contained in the adhesive composition (x). To 100% by mass, more preferably 70 to 100% by mass, and still more preferably 85 to 100% by mass.
  • the content of the adhesive resin is preferably 35 to 100% by mass, more preferably 50 to 100% by mass, still more preferably relative to the total amount (100% by mass) of the active ingredients of the adhesive composition (x). It is 60 to 98% by mass, more preferably 70 to 95% by mass.
  • the pressure-sensitive adhesive composition (x) when the pressure-sensitive adhesive composition (x) contains a pressure-sensitive adhesive resin having a functional group, the pressure-sensitive adhesive composition (x) preferably further contains a crosslinking agent.
  • the said crosslinking agent reacts with the adhesive resin which has a functional group, and bridge
  • crosslinking agent examples include an isocyanate crosslinking agent, an epoxy crosslinking agent, an aziridine crosslinking agent, and a metal chelate crosslinking agent. These crosslinking agents may be used independently and may use 2 or more types together. Among these crosslinking agents, an isocyanate-based crosslinking agent is preferable from the viewpoints of increasing cohesive force and improving adhesive force and availability.
  • the content of the crosslinking agent is appropriately adjusted depending on the number of functional groups that the adhesive resin has, but is preferably 0.01 to 10 parts by mass with respect to 100 parts by mass of the adhesive resin having a functional group, The amount is more preferably 0.03 to 7 parts by mass, still more preferably 0.05 to 5 parts by mass.
  • the pressure-sensitive adhesive composition (x) may further contain a tackifier from the viewpoint of further improving the adhesive strength.
  • the “tackifier” is a component that assists in improving the adhesive strength of the above-mentioned adhesive resin, and refers to an oligomer having a mass average molecular weight (Mw) of less than 10,000. It is distinguished from a functional resin.
  • the mass average molecular weight (Mw) of the tackifier is preferably 400 to 10000, more preferably 500 to 8000, and still more preferably 800 to 5000.
  • Examples of the tackifier are obtained by copolymerizing C5 fractions such as rosin resin, terpene resin, styrene resin, pentene, isoprene, piperine, 1,3-pentadiene generated by thermal decomposition of petroleum naphtha.
  • C9 petroleum resin obtained by copolymerizing C9 fractions such as indene generated by thermal decomposition of petroleum naphtha and vinyltoluene, and hydrogenated resins obtained by hydrogenating these.
  • the softening point of the tackifier is preferably 60 to 170 ° C, more preferably 65 to 160 ° C, and still more preferably 70 to 150 ° C.
  • the “softening point” of the tackifier means a value measured according to JIS K2531.
  • a tackifier may be used independently and may use together 2 or more types from which a softening point and a structure differ. And when using 2 or more types of several tackifier, it is preferable that the weighted average of the softening point of these several tackifiers belongs to the said range.
  • the content of the tackifier is preferably 0.01 to 65% by mass, more preferably 0.1 to 50% by mass, based on the total amount (100% by mass) of the active ingredients of the adhesive composition (x). More preferably, it is 1 to 40% by mass, and still more preferably 2 to 30% by mass.
  • the pressure-sensitive adhesive composition (x) contains an additive for pressure-sensitive adhesives used for general pressure-sensitive adhesives in addition to the above-mentioned additives, as long as the effects of the present invention are not impaired. You may do it.
  • an adhesive additive include antioxidants, softeners (plasticizers), rust inhibitors, pigments, dyes, retarders, reaction accelerators (catalysts), ultraviolet absorbers, antistatic agents, and the like. Is mentioned.
  • These pressure-sensitive adhesive additives may be used alone or in combination of two or more.
  • each pressure-sensitive adhesive additive is preferably 0.0001 to 20 parts by mass, more preferably 0.001 to 100 parts by mass of the adhesive resin. ⁇ 10 parts by mass.
  • the first pressure-sensitive adhesive layer (X1) and the second pressure-sensitive adhesive layer (X2) are both non-expandable pressure-sensitive adhesive layers, but preferably do not substantially contain expandable particles.
  • substantially does not contain expandable particles means that the first pressure-sensitive adhesive layer (X1) and the second pressure-sensitive adhesive layer (X2) do not contain expandable particles for a specific purpose. It means that. Therefore, it does not exclude the aspect in which expandable particles are mixed as impurities in the first pressure-sensitive adhesive layer (X1) and the second pressure-sensitive adhesive layer (X2).
  • a release material may be further laminated on the pressure-sensitive adhesive surfaces of the first pressure-sensitive adhesive layer (X1) and the second pressure-sensitive adhesive layer (X2).
  • a release material a release sheet that has been subjected to a double-sided release process, a release sheet that has been subjected to a single-sided release process, or the like is used, and examples include a release material coated on a release material.
  • Examples of the base material for the release material include papers such as high-quality paper, glassine paper, and kraft paper; polyester resin films such as polyethylene terephthalate resin, polybutylene terephthalate resin, and polyethylene naphthalate resin; and olefins such as polypropylene resin and polyethylene resin.
  • a plastic film such as a resin film;
  • release agent examples include silicone-based resins, olefin-based resins, isoprene-based resins, rubber-based elastomers such as butadiene-based resins, long-chain alkyl-based resins, alkyd-based resins, and fluorine-based resins.
  • the thickness of the release material is not particularly limited, but is preferably 10 to 200 ⁇ m, more preferably 25 to 170 ⁇ m, and still more preferably 35 to 80 ⁇ m.
  • the production method of the present invention is a method for producing a cured encapsulant using the above-mentioned pressure-sensitive adhesive sheet, and includes the following steps (1) to (3).
  • -Process (1) The process of sticking the adhesion surface of a 1st adhesive layer (X1) on a hard support body, and mounting a sealing target object on a part of adhesion surface of a 2nd adhesive layer (X2).
  • Step (2) The sealing object and the adhesive surface of the second pressure-sensitive adhesive layer (X2) at least in the periphery of the sealing object are covered with a sealing material, and the sealing material is cured.
  • Step (3) The expandable particles are expanded and the hard support and the first pressure-sensitive adhesive layer (X1) are stacked while the cured sealing body is laminated on the second pressure-sensitive adhesive layer (X2). Separating at the interface P.
  • FIG. 2 is a schematic cross-sectional view in steps (1) to (3) of the method for producing a cured encapsulated body of the present invention.
  • steps (1) to (3) will be described with reference to FIG. 2 as appropriate.
  • Fig.2 (a) is a cross-sectional schematic diagram in process (1) at the time of using the adhesive sheet 1a shown to Fig.1 (a).
  • step (1) as shown in FIG. 2 (a), the adhesive surface of the first adhesive layer (X1) of the adhesive sheet 1a is affixed to the hard support 50, and the adhesive of the second adhesive layer (X2).
  • the sealing object 60 is placed on a part of the surface.
  • the number of sealing objects to be placed on a part of the adhesive surface of the second pressure-sensitive adhesive layer (X2) may be one or plural as shown in FIG. .
  • FIG. 2 although the aspect using the adhesive sheet 1a shown to Fig.1 (a) is shown, also when using the adhesive sheet which has another structure, a hard support body, an adhesive sheet, And the semiconductor chip are stacked or placed in this order, the adhesive surface of the first adhesive layer (X1) of the adhesive sheet is attached to the hard support, and the adhesive surface of the second adhesive layer (X2) is sealed. It is preferable to affix to the exposed surface of the object.
  • the step (1) may be performed under a temperature condition that is lower than the expansion start temperature (t) of the thermally expandable particles. Is preferably performed in an environment of 0 to 80 ° C. (when the expansion start temperature (t) is 60 to 80 ° C., in an environment lower than the expansion start temperature (t)).
  • the hard support is preferably affixed to the entire pressure-sensitive adhesive surface of the first pressure-sensitive adhesive layer (X1) of the pressure-sensitive adhesive sheet. Therefore, the hard support is preferably plate-shaped. Moreover, it is preferable that the area of the surface of the hard support stuck with the 1st adhesive layer (X1) is more than the area of the adhesive surface of the 1st adhesive layer (X1), as shown in FIG.
  • Examples of the material constituting the hard support include, for example, metal materials such as SUS; non-metallic inorganic materials such as glass and silicon wafers; epoxy resins, ABS resins, acrylic resins, engineering plastics, super engineering plastics, polyimide resins, polyamideimides Examples thereof include resin materials such as resins; composite materials such as glass epoxy resins, and among these, SUS, glass, and silicon wafers are preferable.
  • Examples of engineering plastics include nylon, polycarbonate (PC), and polyethylene terephthalate (PET).
  • Examples of super engineering plastics include polyphenylene sulfide (PPS), polyether sulfone (PES), and polyether ether ketone (PEEK).
  • the thickness of the hard support is preferably 20 ⁇ m or more and 50 mm or less, and more preferably 60 ⁇ m or more and 20 mm or less.
  • the semiconductor chip is sufficiently fixed to the hard support, and the occurrence of positional deviation of the sealing object or the sealing of the sealing object to the exposed surface in the step (2) From the viewpoint of effectively suppressing adverse effects such as resin adhesion, it is preferably 1.0 GPa or more, more preferably 5.0 GPa or more, still more preferably 10 GPa or more, and even more preferably 20 GPa or more.
  • the Young's modulus of the hard support is a value measured at room temperature (25 ° C.) in accordance with the static Young's modulus test method of JIS Z2280: 1993.
  • examples of the sealing object placed on a part of the adhesive surface of the second adhesive layer (X2) include, for example, a semiconductor chip, a semiconductor wafer, a compound semiconductor, a semiconductor package, an electronic component, a sapphire substrate, a display, Panel substrates and the like can be mentioned.
  • the sealing target object mounted may be comprised from the same kind, and may be comprised from 2 or more types of different things.
  • the exposed surface of these objects to be sealed refers to the surface that is in contact with the adhesive surface of the second pressure-sensitive adhesive layer (X2) and is not covered with the sealing material, and specifically corresponds to the circuit surface.
  • the sealing object since the sealing object is sufficiently fixed to the hard support, the sealing resin on the exposed surface of the sealing object is sealed during the sealing step of step (2). It is possible to effectively suppress harmful effects such as adhesion. For example, if the sealing resin adheres to the circuit surface, the circuit wiring is disconnected, which causes a decrease in yield. However, according to the manufacturing method of the present invention, such an adverse effect can be suppressed.
  • Examples of the method for placing the sealing object include a pick-and-place method using an apparatus such as a flip chip bonder and a die bonder, and a batch transfer method using a transfer device. Further, the layout, the number of arrangements, and the like of the objects to be sealed may be appropriately determined according to the target package form, the number of production, and the like.
  • the cured sealing body manufactured by the manufacturing method of the present invention is preferably used for FOWLP. Therefore, it is preferable that the sealing object is a semiconductor chip.
  • a conventionally known semiconductor chip can be used, and a semiconductor chip on which an integrated circuit composed of circuit elements such as a transistor, a resistor, and a capacitor is formed can be used.
  • a semiconductor chip used in one embodiment of the present invention is a semiconductor wafer in which a circuit is formed on one surface of a substrate formed of silicon, SiC (silicon carbide), gallium, arsenic, or the like by an etching method, a lift-off method, or the like. Can be obtained.
  • a stealth dicing method, a tip dicing method, or a method other than these methods may be used as a method of obtaining a semiconductor chip from a semiconductor wafer.
  • the exposed surface of the semiconductor chip placed on the adhesive surface of the second adhesive layer (X2) is preferably a circuit surface on which a circuit is formed.
  • the circuit surface of the semiconductor chip By placing the circuit surface of the semiconductor chip on the adhesive surface of the second pressure-sensitive adhesive layer (X2), the circuit surface of the semiconductor chip can be protected in the process of step (2).
  • the surface opposite to the circuit surface of the semiconductor chip (hereinafter also referred to as “back surface”) is the side that is covered with a sealing material in the next step, and normally, no circuit or electrode is formed. It is a flat surface.
  • the semiconductor chip is placed on a part of the adhesive surface of the second pressure-sensitive adhesive layer (X2), and the plurality of semiconductor chips are arranged in a state of being spaced apart at a certain interval. It is preferable that the plurality of semiconductor chips be mounted on the adhesive surface in a state of being arranged in a matrix of a plurality of rows and a plurality of columns with a certain interval. The interval between the semiconductor chips may be determined as appropriate according to the form of the target package.
  • Step (2) As shown in FIG. 2B, the sealing object 60 and the adhesive surface of the second adhesive layer (X2) at least in the peripheral part of the sealing object 60 are sealed.
  • the sealing material 70 is covered (hereinafter also referred to as “coating treatment”), the sealing material 70 is cured (hereinafter also referred to as “curing treatment”), and the sealing object 60 is sealed with the sealing material 70.
  • coating treatment hereinafter also referred to as “coating treatment”
  • curing treatment hereinafter also referred to as “curing treatment”
  • the sealing material is It is preferable to cover the gap between the objects to be sealed. Moreover, as shown in FIG.2 (b), you may coat
  • the sealing material has a function of protecting the object to be sealed and its accompanying elements from the external environment.
  • the sealing material used in the production method of the present invention is preferably a thermosetting sealing material containing a thermosetting resin from the viewpoint of handleability.
  • the sealing material may be a solid such as a granule, a pellet, or a film at room temperature, or may be a liquid in the form of a composition.
  • a sealing resin film that is a stopper is preferred.
  • the coating method it can select and apply suitably from the methods applied to the conventional sealing process according to the kind of sealing material.
  • Specific examples of the coating method include a roll laminating method, a vacuum pressing method, a vacuum laminating method, a spin coating method, a die coating method, a transfer molding method, and a compression molding method.
  • the coating treatment and the curing treatment in the step (2) are preferably performed in an environment where the expandable particles do not expand.
  • the step (2) may be performed under a temperature condition that is lower than the expansion start temperature (t) of the thermally expandable particles. Is preferably performed in an environment of 0 to 80 ° C. (when the expansion start temperature (t) is 60 to 80 ° C., in an environment lower than the expansion start temperature (t)).
  • the sealing material is hardened and the hardening sealing body formed by sealing a sealing target object with a sealing material is obtained.
  • the coating process and the thermosetting process may be performed separately. However, when the sealing material is heated in the coating process, the sealing material is thermoset as it is by the heating, and the coating process and the heat curing process are performed. You may implement a hardening process simultaneously.
  • Step (3) the expandable particles are expanded, and the cured sealing body is laminated on the second pressure-sensitive adhesive layer (X2), with the hard support and the first pressure-sensitive adhesive layer (X1). This is a process of separation at the interface P.
  • FIG. 2C shows a state where the expandable particles in the expandable base material layer (Y1) are expanded and separated at the interface P between the hard support 50 and the first pressure-sensitive adhesive layer (X1). .
  • the method for expanding the expandable particles is appropriately selected according to the type of the expandable particles.
  • heat treatment is performed at a temperature equal to or higher than the expansion start temperature (t) of the heat-expandable particles to expand the heat-expandable particles.
  • the “temperature higher than the expansion start temperature (t)” is preferably “expansion start temperature (t) + 10 ° C.” or higher and “expansion start temperature (t) + 60 ° C.” or lower. It is more preferable that the temperature is not less than “temperature (t) + 15 ° C.” and not more than “expansion start temperature (t) + 40 ° C.”.
  • the pressure-sensitive adhesive sheet having the expandable base material layer (Y1) containing the expandable particles By forming irregularities on the adhesive surface of (X1), it is adjusted so that it can be separated at the interface P between the hard support and the first adhesive layer (X1). Therefore, the contamination of the hard support, such that a part of the first pressure-sensitive adhesive layer (X1) remains on the surface of the hard support after the separation, can be eliminated, and the washing process of the hard support can be omitted. Can be improved.
  • this step when the expandable particles are expanded, it is preferable not to separate between the layers of the pressure-sensitive adhesive sheet. That is, as shown in FIG. 2 (c), it is preferable to remove all the layers of the pressure-sensitive adhesive sheet without remaining on the surface of the hard support 50 by the step (3).
  • the hard support after separating the pressure-sensitive adhesive sheet is generally subjected to the same process by attaching a new pressure-sensitive adhesive sheet again. At this time, if a part of the pressure-sensitive adhesive sheet remains on the surface of the hard support due to separation between the layers constituting the pressure-sensitive adhesive sheet, a step for removing this layer is required.
  • the first pressure-sensitive adhesive layer (X1) located in the outermost layer of the pressure-sensitive adhesive sheet is a non-intumescent pressure-sensitive adhesive layer. Defects such as the pressure-sensitive adhesive layer (X1) dropping off hardly occur. From this point of view, the problem of contamination in the manufacturing environment is suppressed, which is a factor that can improve productivity.
  • the resulting cured sealing body effectively suppresses adverse effects such as occurrence of displacement of the sealing object and adhesion of the sealing resin to the exposed surface of the sealing object. Has been. Therefore, according to the manufacturing method of this invention, the yield in manufacture of such a hardening sealing body can be improved.
  • the obtained cured encapsulant is thereafter subjected to a step of grinding the encapsulant of the cured encapsulant until the surface of the object to be sealed is exposed, a step of rewiring the circuit surface, an external electrode You may pass through the process of forming a pad and connecting an external electrode pad and an external terminal electrode. Further, after the external terminal electrode is connected to the cured sealing body, it can be separated into individual pieces to manufacture a semiconductor device.
  • the formed heat-expandable base material layer (Y1) was 5 mm long ⁇ 30 mm wide ⁇ 200 ⁇ m thick, and the sample from which the release material was removed was used as a test sample.
  • a dynamic viscoelasticity measuring apparatus TA Instruments, product name “DMAQ800”
  • a test start temperature 0 ° C.
  • a test end temperature 300 ° C.
  • a temperature increase rate of 3 ° C./min a frequency of 1 Hz
  • an amplitude of 20 ⁇ m Under the conditions, the storage elastic modulus E ′ of the test sample at a predetermined temperature was measured.
  • ⁇ Storage shear modulus G ′ of the first pressure-sensitive adhesive layer (X1) and the second pressure-sensitive adhesive layer (X2)> A sample prepared by cutting the formed first pressure-sensitive adhesive layer (X1) and second pressure-sensitive adhesive layer (X2) into a circle having a diameter of 8 mm, removing the release material, and superposing them to obtain a thickness of 3 mm It was.
  • a torsional shear method under conditions of a test start temperature of 0 ° C., a test end temperature of 300 ° C., a heating rate of 3 ° C./min, and a frequency of 1 Hz was used to measure the storage shear modulus G ′ of the test sample at a given temperature.
  • ⁇ Probe tack value> A base material layer to be measured was cut into a square with a side of 10 mm, and then allowed to stand for 24 hours in an environment of 23 ° C. and 50% RH (relative humidity) was used as a test sample. Using a tacking tester (manufactured by Nippon Special Instrument Co., Ltd., product name “NTS-4800”) in an environment of 23 ° C. and 50% RH (relative humidity), the probe tack value on the surface of the test sample was measured according to JIS. It measured based on Z0237: 1991.
  • a stainless steel probe having a diameter of 5 mm is brought into contact with the surface of the test sample at a contact load of 0.98 N / cm 2 for 1 second, and then the probe is moved at a speed of 10 mm / sec. The force required to separate from the surface was measured, and the obtained value was used as the probe tack value of the test sample.
  • Acrylic copolymer (ii): n-butyl acrylate (BA) / methyl methacrylate (MMA) / 2-hydroxyethyl acrylate (HEA) / acrylic acid 86.0 / 8.0 / 5.0 / 1.
  • first pressure-sensitive adhesive layer (X1) To 100 parts by mass of the solid content of the acrylic copolymer (i), which is an adhesive resin, 5.0 parts by mass of the isocyanate-based crosslinking agent (i) ( (Solid content ratio) was mixed, diluted with toluene, and stirred uniformly to prepare a pressure-sensitive adhesive composition having a solid content concentration (active ingredient concentration) of 25% by mass. And the said adhesive composition is apply
  • the 1st adhesive layer (X1) which is an agent layer was formed.
  • the storage shear modulus G ′ (23) of the first pressure-sensitive adhesive layer (X1) at 23 ° C. was 2.5 ⁇ 10 5 Pa.
  • Second pressure-sensitive adhesive layer (X2) To 100 parts by mass of the acrylic copolymer (ii), which is an adhesive resin, 0.8 parts by mass of the isocyanate-based crosslinking agent (i) ( (Solid content ratio) was mixed, diluted with toluene, and stirred uniformly to prepare a pressure-sensitive adhesive composition having a solid content concentration (active ingredient concentration) of 25% by mass. And the said adhesive composition is apply
  • the storage shear modulus G ′ (23) of the second pressure-sensitive adhesive layer (X2) at 23 ° C. was 9.0 ⁇ 10 4 Pa.
  • the adhesive force of the 2nd adhesive layer (X2) measured based on the said method was 1.0 N / 25mm. Since it was clear that the second pressure-sensitive adhesive layer (X2) and the first pressure-sensitive adhesive layer (X1) had a probe tack value of 50 mN / 5 mm ⁇ or more, measurement of the probe tack value was omitted.
  • the resin composition is formed on the surface of a 50 ⁇ m-thick polyethylene terephthalate (PET) film (product name “COSMO SHINE A4100”, probe tack value: 0 mN / 5 mm ⁇ , manufactured by Toyobo Co., Ltd.), which is a non-intumescent substrate.
  • PET polyethylene terephthalate
  • COSMO SHINE A4100 probe tack value: 0 mN / 5 mm ⁇ , manufactured by Toyobo Co., Ltd.
  • the product was applied to form a coating film, and the coating film was dried at 100 ° C. for 120 seconds to form an expandable substrate layer (Y1) having a thickness of 50 ⁇ m.
  • the PET film corresponds to the non-expandable base material layer (Y2).
  • the resin composition is applied to the surface of the release agent layer of the light release film to form a coating film, and the coating film is formed into 100. Drying was performed at ° C for 120 seconds to similarly form an expandable substrate layer (Y1) having a thickness of 50 ⁇ m.
  • the storage elastic modulus and probe tack value in each temperature of an expansible base material layer (Y1) were measured. The measurement results were as follows. -Storage elastic modulus E '(23) at 23 ° C.
  • peel force (F 0) and (F 1) measured in accordance with the following methods.
  • peeling is performed at the interface P between the silicon wafer and the first pressure-sensitive adhesive layer (X1) of the pressure-sensitive adhesive sheet at a pulling speed of 300 mm / min according to JIS Z0237: 2000 by a 180 ° peeling method.
  • the peeling force measured at the time of the measurement was defined as “peeling force (F 0 )”.
  • peeling force (F 1 ) The heavy release film of the prepared pressure-sensitive adhesive sheet is removed, and the exposed first pressure-sensitive adhesive layer (X1) is attached to a silicon wafer, heated at 240 ° C. for 3 minutes, and in the thermally expandable base material layer (Y1). The thermally expandable particles were expanded. Thereafter, in the same manner as the measurement of the peeling force (F 0 ) described above, the peeling force measured when peeling was performed at the interface P between the silicon wafer and the first pressure-sensitive adhesive layer (X1) of the pressure-sensitive adhesive sheet under the above conditions. Was defined as “peeling force (F 1 )”.
  • the adhesive sheet (I) is completely separated from the silicon wafer when the adhesive sheet is fixed with the upper chuck of the universal tensile testing machine and cannot be fixed. The measurement was terminated, and the peeling force (F 1 ) at that time was set to “0 mN / 25 mm”.
  • Example 1 ⁇ Step (1)> The pressure-sensitive adhesive sheet produced in Production Example 2 was cut into a square size of 230 mm ⁇ 230 mm. Using a tape grinder for back grind (manufactured by Lintec Corporation, device name “RAD-3510F / 12”), the heavy release film of the cut adhesive sheet was peeled off, and the first adhesive layer (X1) exposed was exposed. The adhesive surface was attached to a hard support (material: silicon, thickness: 725 ⁇ m, Young's modulus: 30 GPa). Further, the light release film was also peeled off, and nine semiconductor chips (the size of each chip was 6.4 mm long ⁇ 6.4 horizontal) on the adhesive surface of the exposed second pressure-sensitive adhesive layer (X2). X A rectangular parallelepiped shape having a thickness of 200 ⁇ m (# 2000) was placed at a certain interval so that the circuit surface on which the circuit was formed was in contact with the adhesive surface.
  • a tape grinder for back grind manufactured by Lintec Corporation, device name “RAD-3510F /
  • Step (2)> The nine semiconductor chips and the adhesive surface of the second adhesive layer (X2) at least in the periphery of the semiconductor chip are covered with a thermosetting sealing resin film as a sealing material, and heated in a vacuum Using a pressure laminator (“7024HP5” manufactured by ROHM and HAAS), the sealing resin film was thermally cured to produce a cured sealing body formed by sealing the semiconductor chip with a sealing material.
  • the sealing conditions are as follows. -Preheating temperature: 100 ° C for both table and diaphragm ⁇ Vacuum drawing: 60 seconds ⁇ Dynamic press mode: 30 seconds ⁇ Static press mode: 10 seconds ⁇ Sealing temperature: 180 ° C. ⁇ 60 minutes Note that the semiconductor chip is not misaligned when covered with the above sealing resin film. Was not.
  • the surface of the hard support after the pressure-sensitive adhesive sheet is separated is not confirmed to remain in the first pressure-sensitive adhesive layer (X1), is not contaminated, and the surface of the hard support is newly cleaned. It is thought that there is no need to perform the process. Further, the semiconductor chip sealed in the obtained cured sealing body was not misaligned, and no sealing resin was observed on the circuit surface. Furthermore, about the cured sealing body with the pressure-sensitive adhesive sheet after being separated from the hard support, there is no adverse effect such as dropping of the first pressure-sensitive adhesive layer (X1) located in the outermost layer of the pressure-sensitive adhesive sheet. It can be said that the occurrence of contamination is suppressed.

Landscapes

  • Engineering & Computer Science (AREA)
  • Microelectronics & Electronic Packaging (AREA)
  • Chemical & Material Sciences (AREA)
  • General Physics & Mathematics (AREA)
  • Organic Chemistry (AREA)
  • Computer Hardware Design (AREA)
  • Physics & Mathematics (AREA)
  • Power Engineering (AREA)
  • Condensed Matter Physics & Semiconductors (AREA)
  • Manufacturing & Machinery (AREA)
  • Adhesive Tapes (AREA)
  • Adhesives Or Adhesive Processes (AREA)
  • Encapsulation Of And Coatings For Semiconductor Or Solid State Devices (AREA)
  • Laminated Bodies (AREA)
  • Sealing Material Composition (AREA)

Abstract

La présente invention concerne un procédé de production d'un produit d'étanchéité durci à l'aide d'une feuille adhésive comprenant : un matériau de base (Y) équipé d'une couche de matériau de base non expansible (Y2) et d'une couche de matériau de base expansible (Y1) qui contient des particules expansibles ; et une première couche adhésive (X1) et une seconde couche adhésive (X2). Le procédé comprend les étapes (1) à (3). L'étape (1) : une étape consistant à fixer la surface adhésive de la première couche adhésive (X1) à un corps de support dur, et à placer un objet à sceller sur une partie de la surface adhésive de la seconde couche adhésive (X2). L'étape (2) : une étape consistant à recouvrir l'objet à sceller et la surface adhésive de la seconde couche adhésive (X2) avec un agent d'étanchéité, puis à laisser ledit agent d'étanchéité durcir de façon à obtenir un produit d'étanchéité durci. L'étape (3) : une étape consistant à amener les particules expansibles à se dilater de façon à séparer le corps de support dur et la première couche adhésive (X1) l'un de l'autre au niveau d'une interface P entre eux.
PCT/JP2019/020190 2018-06-08 2019-05-22 Procédé de production de produit d'étanchéité durci WO2019235217A1 (fr)

Priority Applications (3)

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JP2020523609A JP7267272B2 (ja) 2018-06-08 2019-05-22 硬化封止体の製造方法
KR1020207035077A KR102727202B1 (ko) 2018-06-08 2019-05-22 경화 봉지체의 제조 방법
CN201980038938.3A CN112262459A (zh) 2018-06-08 2019-05-22 固化密封体的制造方法

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JP2018110617 2018-06-08
JP2018-110617 2018-06-08

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WO2022054889A1 (fr) * 2020-09-14 2022-03-17 リンテック株式会社 Feuille adhésive et procédé de production d'un dispositif à semi-conducteur

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JP2003064329A (ja) * 2001-08-30 2003-03-05 Nitto Denko Corp エネルギー線硬化型熱剥離性粘着シート、これを用いた切断片の製造方法、及びその切断片
WO2013011850A1 (fr) * 2011-07-15 2013-01-24 日東電工株式会社 Procédé de fabrication d'un composant électronique et film adhésif utilisé dans le procédé de fabrication d'un composant électronique

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JP2005101628A (ja) * 2004-10-25 2005-04-14 Nitto Denko Corp 電子部品用加熱剥離型粘着シートおよび電子部品の加工方法並びに電子部品
EP2832812A1 (fr) * 2013-07-29 2015-02-04 Nitto Shinko Corporation Produit d'étanchéité
JP6320239B2 (ja) * 2013-09-24 2018-05-09 日東電工株式会社 半導体チップ封止用熱硬化性樹脂シート及び半導体パッケージの製造方法
JP2017002190A (ja) * 2015-06-10 2017-01-05 リンテック株式会社 加熱剥離性粘着シート
WO2018003312A1 (fr) * 2016-06-30 2018-01-04 リンテック株式会社 Feuille de traitement semi-conducteur

Patent Citations (2)

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Publication number Priority date Publication date Assignee Title
JP2003064329A (ja) * 2001-08-30 2003-03-05 Nitto Denko Corp エネルギー線硬化型熱剥離性粘着シート、これを用いた切断片の製造方法、及びその切断片
WO2013011850A1 (fr) * 2011-07-15 2013-01-24 日東電工株式会社 Procédé de fabrication d'un composant électronique et film adhésif utilisé dans le procédé de fabrication d'un composant électronique

Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO2022054889A1 (fr) * 2020-09-14 2022-03-17 リンテック株式会社 Feuille adhésive et procédé de production d'un dispositif à semi-conducteur

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CN112262459A (zh) 2021-01-22
TW202000822A (zh) 2020-01-01
JP7267272B2 (ja) 2023-05-01
KR20210018272A (ko) 2021-02-17
JPWO2019235217A1 (ja) 2021-07-08

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