JP2013199103A - Laminate and cutting laminate - Google Patents

Abstract

PROBLEM TO BE SOLVED: To provide a laminate that can suppress adhesion of foreign matters to an insulating layer, and in addition can easily peel off the insulating layer from a protective film layer.SOLUTION: A laminate 1 includes: a thermal conductor 2 whose thermal conductivity is ≥10 W/m K; an insulating layer 3 laminated on the surface of the thermal conductor 2; and a protective film layer 4 laminated on the surface opposite to the thermal conductor 2 side of the insulating layer 3. The protective film layer 4 has a base material 4A and a sticking part 4B laminated on the surface of the base material 4A. The protective film layer 4 is laminated on the surface of the insulating layer 3 from the sticking part 4B side. The protective film layer 4 has an irregular shape in the surface of the insulating layer 3 side of the sticking part 4B.

Description

  The present invention relates to a laminate including a heat conductor having a thermal conductivity of 10 W / m · K or more and an insulating layer. The present invention also relates to a cut laminate using the laminate. Moreover, this invention relates to the manufacturing method of the components for power semiconductor modules using this laminated body.

  In recent years, miniaturization and high performance of electric devices have been advanced. Along with this, the mounting density of electronic components is increasing, and the need to dissipate heat generated from electronic components is increasing. As a method of dissipating heat, a method of adhering a heat conductor having high heat dissipation and a thermal conductivity of 10 W / m · K or more to a heat generation source is widely adopted. In addition, an insulating adhesive material having an insulating property is used to bond the heat conductor to a heat source.

  An example of an electrical device using the insulating adhesive material is disclosed in Patent Document 1 below. In Patent Document 1, an insulating resin layer having a thermal conductivity of 1.0 to 7.5 W / (m · K) and a thickness of 50 to 150 μm is provided on one main surface of a plate-shaped metal heat sink. There is disclosed a circuit board for a semiconductor power module having a metal insulating plate provided and configured, and a lead frame provided on the insulating resin layer of the metal insulating plate. The lead frame has a stepped bent portion. The bent portion is located 2 mm or more inward from the end of the main surface of the heat sink, and is bent so that the floating dimension of the lead frame at the end of the heat sink is 1 mm or more. The metal insulating plate and the lead frame are press-bonded via an adhesive resin layer having a thickness of 10 to 50 μm.

  In Patent Document 1 below, as a method for producing the metal insulating plate, an epoxy resin in which a silicon oxide filler is dispersed is formed into a sheet, and then press laminated on a 2 mm thick aluminum plate to be a heat sink. A method for producing the metal insulating plate by punching is described.

Japanese Patent No. 3846699

  In Patent Document 1, when manufacturing the metal insulating plate, surrounding dust or metal wear powder generated during processing may adhere to the insulating layer.

  The object of the present invention is to provide a protective film layer, thereby suppressing adhesion of foreign matter to the insulating layer, and further using the laminated body that can easily peel the protective film layer from the insulating layer. It is to provide a cut laminate.

  Another object of the present invention is to provide a method for manufacturing a power semiconductor module component that can suppress adhesion of foreign matter to the insulating layer because the protective film layer is provided, and that the protective film layer can be favorably peeled from the insulating layer. Is to provide.

  According to a wide aspect of the present invention, a thermal conductor having a thermal conductivity of 10 W / m · K or more, an insulating layer laminated on a surface of the thermal conductor, the thermal conductor side of the insulating layer, A protective film layer laminated on the opposite surface, wherein the protective film layer has a base material and an adhesive part laminated on the surface of the base material, and the protective film layer is on the adhesive part side To the surface of the insulating layer, and the protective film layer has a concavo-convex shape on the surface of the adhesive portion on the insulating layer side.

  Moreover, according to the wide situation of this invention, the manufacturing method of the components for power semiconductor modules using the laminated body mentioned above is provided.

  That is, according to a wide aspect of the present invention, a thermal conductor having a thermal conductivity of 10 W / m · K or more, an insulating layer laminated on a surface of the thermal conductor, and the thermal conduction of the insulating layer A protective film layer laminated on a surface opposite to the body side, wherein the protective film layer has a base material and an adhesive portion laminated on the surface of the base material, and the protective film A layer is laminated on the surface of the insulating layer from the pressure-sensitive adhesive portion side, and the protective film layer is formed by using a laminate having a concavo-convex shape on the surface of the pressure-sensitive adhesive portion on the insulating layer side. Peeling the protective film layer from the surface, laminating a conductive layer on the exposed surface of the insulating layer, curing the insulating layer, the thermal conductor, the insulating layer, and the conductive layer. And a process of embedding in a mold resin Method for producing parts for the body module is provided.

  In this specification, both the invention relating to the above-described laminate and the invention relating to the above-described method for manufacturing a module component for a power semiconductor device are disclosed.

  It is preferable that the surface on the insulating layer side of the adhesive portion is embossed. It is preferable that the protective film layer does not have an uneven shape on the surface opposite to the adhesive portion side of the base material. The ratio of the thickness of the protective film layer to the thickness of the insulating layer is preferably 0.2 or more and 1 or less. The ten-point average roughness Rz of the surface of the adhesive portion on the insulating layer side is preferably 1 μm or more and 50 μm or less. The protective film layer is preferably colored.

  The insulating layer preferably contains an inorganic filler having a thermal conductivity of 10 W / m · K or more. It is preferable that the insulating layer has a plurality of layers having different curing rates and is a multilayer. It is preferable that the curing rate of the surface of the insulating layer on the protective film layer side is 20% or more and 80% or less.

  The material of the substrate is preferably a polyester resin.

  According to a wide aspect of the present invention, there is provided a cut laminate obtained by cutting the above-described laminate in a state where the heat conductor, the insulating layer, and the protective film layer are laminated. .

  The cut laminate according to the present invention is preferably obtained by cutting the above-described laminate by press punching.

  In a specific aspect of the method for manufacturing a power semiconductor module component according to the present invention, the laminate is obtained by cutting the laminated body in a state where the thermal conductor, the insulating layer, and the protective film layer are laminated. Using the cut laminate, the protective film layer is peeled off from the surface of the insulating layer, and a conductive layer is stacked on the exposed surface of the insulating layer. In this case, it is preferable to cut the laminate by press punching.

  The laminate according to the present invention includes a thermal conductor having a thermal conductivity of 10 W / m · K or more, an insulating layer laminated on the surface of the thermal conductor, and the opposite side of the insulating layer to the thermal conductor side. Since the protective film layer laminated | stacked on the surface of this is provided, it can suppress that a foreign material adheres to an insulating layer.

  Furthermore, the protective film layer has a base material and an adhesive part laminated on the surface of the base material, the protective film layer is laminated on the surface of the insulating layer from the adhesive part side, Since the said protective film layer has an uneven | corrugated shape in the surface by the side of the said insulating layer of the said adhesion part, a protective film layer can be peeled favorably from an insulating layer.

  In the method for manufacturing a power semiconductor module according to the present invention, since the laminate is used, adhesion of foreign matters to the insulating layer can be suppressed, and the protective film layer can be favorably peeled from the insulating layer. Moreover, as a result of being able to peel the protective film layer from the insulating layer satisfactorily, a good power semiconductor module component can be obtained.

FIG. 1 is a cross-sectional view schematically showing a laminate according to an embodiment of the present invention. FIG. 2 is a cross-sectional view schematically showing a power semiconductor module component obtained using the laminate according to the embodiment of the present invention.

  The laminate according to the present invention includes a thermal conductor having a thermal conductivity of 10 W / m · K or more, an insulating layer laminated on the surface of the thermal conductor, and the opposite side of the insulating layer to the thermal conductor side. And a protective film layer laminated on the surface. The said protective film layer has a base material and the adhesion part laminated | stacked on the surface of this base material. The said protective film layer is laminated | stacked on the surface of the said insulating layer from the said adhesion part side. The protective film layer has a concavo-convex shape on the surface of the adhesive portion on the insulating layer side.

  By adopting the above-described configuration in the laminate according to the present invention, the protective film layer is laminated on the surface of the insulating layer, thereby preventing foreign matter from adhering to the insulating layer. For example, it is possible to suppress adhesion of foreign matters such as surrounding dust and metal wear powder generated during processing to the insulating layer. In particular, when the laminated body is cut into a predetermined size in a state where the thermal conductor, the insulating layer, and the protective film layer are laminated, a cut piece or a broken piece of a cutting blade used at the time of cutting, etc. The adhesion of foreign matter is suppressed.

  Furthermore, in the laminated body which concerns on this invention, since the said protective film layer has an uneven | corrugated shape on the surface by the side of the said insulating layer of the said adhesion part, a protective film layer can be peeled favorably from an insulating layer. In particular, when the laminated body is cut into a predetermined size by press punching in a state where the thermal conductor, the insulating layer, and the protective film layer are laminated, the protective film layer is strongly attached to the insulating layer by pressure. There is a problem. On the other hand, the protective film layer has an uneven shape on the surface of the adhesive portion on the insulating layer side, so that the protective film layer can be separated from the insulating layer even after the laminate is cut by press punching. It can peel well.

  In the method for manufacturing a power semiconductor module component according to the present invention, the above-described laminate is used. In the method for manufacturing a power semiconductor module component according to the present invention, the protective film layer is peeled off from the surface of the insulating layer, and a conductive layer is stacked on the exposed surface of the insulating layer, using the laminate described above. A step, a step of curing the insulating layer, and a step of embedding the thermal conductor, the insulating layer, and the conductive layer in a mold resin.

  Adoption of the above-described configuration in the method for manufacturing a power semiconductor module component according to the present invention can prevent foreign matter from adhering to the insulating layer. For example, it is possible to suppress adhesion of foreign matters such as surrounding dust and metal wear powder generated during processing to the insulating layer. In particular, when the laminated body is cut into a predetermined size in a state where the thermal conductor, the insulating layer, and the protective film layer are laminated, a cut piece or a broken piece of a cutting blade used at the time of cutting, etc. The adhesion of foreign matter is suppressed.

  Furthermore, in the method for manufacturing a component for a power semiconductor module according to the present invention, the protective film layer has a concavo-convex shape on the surface of the adhesive portion on the insulating layer side, and thus the protective film layer is peeled off from the insulating layer satisfactorily Can do. In particular, in a state where the thermal conductor, the insulating layer, and the protective film layer are laminated, the protective film layer is excellent from the insulating layer even after the laminate is cut into a predetermined size by press punching. Can be peeled off. Moreover, as a result of being able to peel the protective film layer from the insulating layer satisfactorily, a good power semiconductor module component can be obtained.

  In the present invention, a protective film layer having a base material and an adhesive portion and having an uneven shape on the surface of the adhesive portion is laminated on the surface of the insulating layer in a laminated state of the thermal conductor and the insulating layer. Therefore, a new configuration that has not been conventionally used is employed. In order to easily peel the protective film layer from the surface of the insulating layer, it is conceivable to reduce the adhesive strength of the adhesive portion instead of forming an uneven shape on the surface of the adhesive portion. However, when the adhesive strength of the adhesive portion in the protective film layer is lowered, the protective film layer is easily peeled off from the insulating layer when the laminate is cut. By using a protective film layer having a concavo-convex shape on the surface of the pressure-sensitive adhesive part, the protective film layer can be peeled off well from the insulating layer during use of the laminate, and can also be protected during processing of the laminate. Unintentional peeling of the film layer from the insulating layer can also be suppressed.

  In addition, the present inventors manufactured electronic parts such as a plurality of power semiconductor module parts by using a laminate, because the protective film layer has an uneven shape on the surface of the adhesive part on the insulating layer side. In some cases, it was found that variations in withstand voltage among a plurality of insulating layers can be reduced. In the present invention, the variation in the voltage resistance among the plurality of insulating layers is reduced, and as a result, a homogeneous electronic component such as a power semiconductor module component can be manufactured.

  In the laminated body, the surface of the insulating layer opposite to the heat conductor side is preferably a surface laminated on the conductive layer. The laminate is preferably a laminate used by laminating a conductive layer on the surface of the insulating layer opposite to the thermal conductor side.

  The laminated body is preferably a laminated body that is cut and used in a state in which the thermal conductor, the insulating layer, and the protective film layer are laminated. The laminated body is preferably a laminated body used by being cut by press punching in a state where the thermal conductor, the insulating layer, and the protective film layer are laminated.

  The cut laminated body according to the present invention is obtained by cutting the laminated body in a state in which the thermal conductor, the insulating layer, and the protective film layer are laminated. At this time, the laminate is cut into a predetermined size. The cut laminate according to the present invention is preferably obtained by cutting the laminate by press punching in a state where the heat conductor, the insulating layer, and the protective film layer are laminated. Even if such cutting is performed, it is possible to suppress the adhesion of foreign matter to the insulating layer, and further, the protective film layer can be peeled off from the insulating layer after cutting.

  Moreover, in the manufacturing method of the component for power semiconductor modules which concerns on this invention, the laminated body obtained by cut | disconnecting the said laminated body in the state in which the said heat conductor, the said insulating layer, and the said protective film layer were laminated | stacked. It is preferable that the protective film layer is peeled off from the surface of the insulating layer using a body and a conductive layer is laminated on the exposed surface of the insulating layer. In this case, it is preferable to cut the laminate by press punching.

  It does not specifically limit as a method of forming the said uneven | corrugated shape, For example, an embossing roll method, a calender roll method, a profile extrusion method, etc. are mentioned. Among them, the embossing roll method is preferable because it can form a large number of concavo-convex embossments that are quantitatively constant. The surface of the adhesive portion on the insulating layer side is preferably embossed. That is, it is preferable that the uneven shape is given by embossing.

  The method for forming the concavo-convex shape is not particularly limited, and a method of passing a protective film heated to a predetermined temperature between embossing rolls heated to a predetermined temperature to impart a concavo-convex shape to the surface, an uncured adhesive Examples of the method include curing in a state where the portion is in close contact with a roll or sheet having an embossed structure, and transferring the embossed structure.

  It is preferable that the protective film layer does not have a concavo-convex shape on the surface opposite to the adhesive portion side of the base material layer. In this case, the protective film layer can be peeled off more favorably from the surface of the insulating layer, and even after the laminate is cut by press punching or the like, the protective film layer is further improved from the insulating layer. Can be peeled off. However, the said protective film layer may have an uneven | corrugated shape on the surface on the opposite side to the said adhesion part side of the said base material layer.

  The ratio (T1 / T2) of the thickness (T1) of the protective film layer to the thickness (T2) of the insulating layer is preferably 0.05 or more, more preferably 0.1 or more, still more preferably 0.2 or more, preferably Is 20 or less, more preferably 10 or less, and still more preferably 1 or less. The ratio (T1 / T2) is particularly preferably 0.2 or more and 1 or less. When the ratio (T1 / T2) is not less than the above lower limit and not more than the above upper limit, the peelability of the protective film layer is further improved. The thickness (T1) of the protective film layer is the total thickness of the base material and the adhesive portion.

  The ten-point average roughness Rz of the surface on the insulating layer side of the protective film layer and the ten-point average roughness Rz of the surface on the insulating layer side of the adhesive part are each preferably 1 μm or more, preferably 100 μm or less, More preferably, it is 70 micrometers or less, More preferably, it is 60 micrometers or less, Most preferably, it is 50 micrometers or less. The ten-point average roughness Rz is particularly preferably 1 μm or more and 50 μm or less. When the ten-point average roughness Rz is not less than the above lower limit and not more than the above upper limit, the protective film layer can be peeled off more favorably from the surface of the insulating layer, and further after the laminate is cut by press punching or the like Even if it exists, a protective film layer can be peeled more favorably from an insulating layer, and also stability of withstand voltage can be improved further. The ten-point average roughness Rz is measured according to JIS B0601-1994.

  The protective film layer is preferably colored. In this case, the visibility of the protective film is improved, and it is easy to find a defect when, for example, a peeling failure occurs during the manufacturing process or a protective film layer is dropped during punching. When the protective film layer is colored, the base material may be colored, the adhesive part may be colored, or both the base material and the adhesive part may be colored.

  Examples of the material of the base material include polyester resins such as polyethylene terephthalate (PET) resin, polytetrafluoroethylene resin, polyethylene (PE) resin, polypropylene resin, polymethylpentene resin, polyolefin resin such as polyvinyl acetate resin, and polyvinyl chloride. Examples thereof include resins and polyimide resins. The material of the substrate is preferably a polyester resin. By using the base material formed of the polyester resin, the peelability of the protective film layer is further improved.

  The material of the said adhesion part is not specifically limited. Examples of the material of the adhesive part include acrylic adhesives, special synthetic rubber adhesives, synthetic resin adhesives, silicone adhesives, rubber adhesives, and the like.

  The thickness of the protective film layer is preferably 10 μm or more, more preferably 20 μm or more, preferably 200 μm or less, more preferably 150 μm or less. The thickness of the adhesive part is preferably 1 μm or more, more preferably 3 μm or more, preferably 100 μm or less, more preferably 50 μm or less. It is preferable that the thickness of the adhesive part exceeds the concave part depth or convex part height in the concave-convex shape.

  The insulating layer has a plurality of layers with different curing rates, and is preferably a multilayer. However, the insulating layer may be a single layer. The insulating layer preferably includes a first insulating layer disposed on the heat conductor side and a second insulating layer disposed on the protective film layer side. The laminated body includes the thermal conductor, a first insulating layer laminated on a surface of the thermal conductor, and a second laminated on a surface opposite to the thermal conductor side of the first insulating layer. And a protective film layer laminated on the surface of the second insulating layer opposite to the first insulating layer side. In this manner, by making the insulating layer into a multilayer, it is possible to impart partially different properties to the insulating layer.

  The curing rate of the surface of the insulating layer on the protective film layer side is preferably 1% or more, and may be 10% or more. The curing rate of the second insulating layer is preferably 1% or more, and may be 10% or more.

  The curing rate of the surface of the insulating layer on the protective film layer side is preferably 20% or more and 80% or less. It is preferable that the curing rate of the surface laminated | stacked on the conductive layer of the said insulating layer is 20% or more and 80% or less. It is preferable that the curing rate of the second insulating layer is 20% or more and 80% or less. In this case, the adhesion between the insulating layer and the conductive layer can be effectively increased. Further, as a result of the surface on the protective film layer side of the insulating layer having a certain hardness and flexibility, the protective film layer is removed from the surface of the insulating layer due to the influence of the uneven shape on the insulating layer side of the protective film layer. Even after the laminate is cut by press punching or the like, the protective film layer can be peeled off better from the insulating layer, and the resistance in the plurality of insulating layers can be further improved. The variation in voltage characteristics can be further reduced.

  It is preferable that the curing rate of the surface on the heat conductor side of the insulating layer is larger than the curing rate of the surface of the insulating layer on the protective film layer side. It is preferable that the curing rate of the first insulating layer is larger than the curing rate of the second insulating layer. In this case, the voltage resistance of the insulating layer can be further effectively improved.

  The curing rate of the surface of the insulating layer on the protective film layer side may be less than 70%, less than 60%, or less than 50%. The curing rate of the second insulating layer is preferably 1% or more, may be less than 70%, may be less than 60%, or may be less than 50%.

  The curing rate of the surface on the heat conductor side of the insulating layer is preferably 50% or more, more preferably 60% or more, still more preferably 70% or more, may be 80% or more, and may be 90% or more. It may be 95% or more, or 100%. The curing rate of the first insulating layer is preferably 50% or more, more preferably 60% or more, still more preferably 70% or more, may be 80% or more, and may be 90% or more. 95% or more, or 100%.

  The second insulating layer is preferably an uncured product or a semi-cured product. The second insulating layer may be an uncured material that is not cured at all and can be cured, or may be a semi-cured material that has been cured and can be further cured. The first insulating layer is preferably a semi-cured product or a cured product. The first insulating layer may be a semi-cured product that has been cured and can be further cured, or a cured product that has been cured.

  From the viewpoint of improving both the thermal conductivity of the entire insulating layer and the adhesion between the insulating layer and the conductive layer in a well-balanced manner, the curing rate of the surface of the insulating layer on the side of the heat conductor is the above-described ratio of the insulating layer. It is preferably 1% or more larger than the curing rate of the surface on the protective film layer side, more preferably 5% or more, further preferably 10% or more, more preferably 20% or more, and 30% or more. Also good. From the viewpoint of improving both the thermal conductivity of the entire insulating layer and the adhesion between the insulating layer and the conductive layer in a balanced manner, the curing rate of the first insulating layer is the curing rate of the second insulating layer. Is preferably 1% or more, more preferably 5% or more, still more preferably 10% or more, and may be 20% or more, or 30% or more.

  The curing rate of the insulating layer is determined by measuring the heat of curing when the uncured insulating layer is heated. When measuring the curing rate, for example, a differential scanning calorimetry (DSC) apparatus (“DSC7020” manufactured by SII Nanotechnology) or the like is used. Specifically, the curing rate of the insulating layer is measured as follows.

  At a measurement start temperature of 30 ° C. and a temperature increase rate of 3 ° C./min, the insulating layer (such as the first insulating layer or the second insulating layer) is heated to 300 ° C. and held for 1 hour. The amount of heat generated when the insulating layer is cured at this temperature rise (hereinafter referred to as heat amount A) is measured. In addition, a curable composition for forming an insulating layer was applied to a release PET (polyethylene terephthalate) sheet having a thickness of 50 μm so as to have a thickness of 80 μm, and 1 ° C. under a room temperature vacuum of 23 ° C. and 0.01 atm. An uncured insulating layer dried without heating is prepared in the same manner as the insulating layer in the above laminate except that it is dried for a period of time. Using this insulating layer, the amount of heat (hereinafter, referred to as the amount of heat B) generated when the temperature is hardened is measured in the same manner as the measurement of the amount of heat A described above. From the obtained heat quantity A and heat quantity B, the curing rates of the first and second insulating layers are obtained by the following formula.

Curing rate (%) = [1- (heat amount A / heat amount B)] × 100
The ratio of the thickness of the second insulating layer to the thickness of the first insulating layer (the thickness of the second insulating layer / the thickness of the first insulating layer) is preferably 0.03 or more, more preferably 0.00. 1 or more, more preferably 0.3 or more, preferably 10 or less, more preferably 3 or less, still more preferably 1 or less.

  From the viewpoint of improving both the thermal conductivity of the entire insulating layer and the adhesion between the second insulating layer, which is a cured product, and the conductive layer in a well-balanced manner, the thickness of the first insulating layer is the first thickness. The ratio of the insulating layer to the thickness is particularly preferably 0.3 or more and 1 or less.

  The thickness of the insulating layer (the entire insulating layer) is not particularly limited. The thickness of the insulating layer is preferably 80 μm or more, more preferably 100 μm or more, preferably 200 μm or less, more preferably 170 μm or less. When the thickness of the insulating layer is equal to or more than the above lower limit, heat dissipation in the entire insulating layer, adhesion between the insulating layer and the conductive layer, which is a cured product, and voltage resistance in the entire insulating layer are improved in a well-balanced manner.

  The insulating layer is preferably formed using a curable compound (A) and a curing agent (B). The first insulating layer is preferably formed using a first curable composition containing a curable compound (A) and a curing agent (B). It is preferable that the said 2nd insulating layer is formed using the 2nd curable composition containing a sclerosing | hardenable compound (A) and a hardening | curing agent (B). From the viewpoint of forming an insulating layer with good curability, the insulating layer is preferably formed using a curable compound (A1) having a cyclic ether group and a curing agent (B). Each of the insulating layer and the curable composition preferably contains an inorganic filler (C). Each of the first insulating layer and the first curable composition preferably contains an inorganic filler (C). Each of the second insulating layer and the second curable composition preferably contains an inorganic filler (C). The inorganic filler (C) is preferably an inorganic filler having a thermal conductivity of 10 W / m · K or more.

  The insulating layer preferably includes an inorganic filler having a thermal conductivity of 10 W / m · K or more. In this case, the thermal conductivity of the insulating layer is increased and the heat dissipation is increased. However, each of the insulating layer, the first insulating layer, and the second insulating layer may include an inorganic filler having a thermal conductivity of less than 10 W / m · K.

  Hereinafter, first, details of each component used for the insulating layer will be described.

(Curable compound (A))
The insulating layer is preferably formed using a curable compound (A). The said curable composition contains a sclerosing | hardenable compound (A). The curable compound (A) is preferably a thermosetting compound. The curable compound (A) is preferably a curable compound (A1) having a cyclic ether group. Examples of the cyclic ether group include an epoxy group and an oxetanyl group. The curable compound (A1) having a cyclic ether group is preferably a curable compound having an epoxy group or an oxetanyl group. The curable compound (A) is cured by the action of the curing agent (B). As for the curable compound (A) used for an insulating layer, only 1 type may be used and 2 or more types may be used together. The curable compound (A) used for the first insulating layer and the curable compound (A) used for the second insulating layer may be the same or different.

  The curable compound (A1) may contain an epoxy compound (A1a) having an epoxy group, or may contain an oxetane compound (A1b) having an oxetanyl group.

  From the viewpoint of further improving the heat resistance and voltage resistance of an insulating layer that is a cured product (hereinafter sometimes simply referred to as a cured product), the curable compound (A) preferably has an aromatic skeleton. From the viewpoint of further improving the thermal conductivity and voltage resistance of the cured product, the curable compound (A) preferably includes a curable compound having a polycyclic aromatic skeleton, and includes a cyclic ether group and a polycyclic ring. It is more preferable to include a curable compound having a formula aromatic skeleton. Examples of the polycyclic aromatic skeleton include a naphthalene skeleton, an anthracene skeleton, a xanthene skeleton, a fluorene skeleton, and a biphenyl skeleton. From the viewpoint of further improving the thermal conductivity and voltage resistance of the cured product, the polycyclic aromatic skeleton is preferably a biphenyl skeleton.

  The content of the curable compound having a polycyclic aromatic skeleton in the total 100% by weight of the curable compound (A) is preferably 30% by weight or more, more preferably 50% by weight or more, and further preferably 60% by weight. That's it. The total amount of the curable compound (A) may be a curable compound having a polycyclic aromatic skeleton.

  Specific examples of the epoxy compound (A1a) having an epoxy group include an epoxy monomer having a bisphenol skeleton, an epoxy monomer having a dicyclopentadiene skeleton, an epoxy monomer having a naphthalene skeleton, an epoxy monomer having an adamantane skeleton, and an epoxy having a fluorene skeleton. Examples of the monomer include an epoxy monomer having a biphenyl skeleton, an epoxy monomer having a bi (glycidyloxyphenyl) methane skeleton, an epoxy monomer having a xanthene skeleton, an epoxy monomer having an anthracene skeleton, and an epoxy monomer having a pyrene skeleton. These hydrogenated products or modified products may be used. As for an epoxy compound (A1a), only 1 type may be used and 2 or more types may be used together.

  Examples of the epoxy monomer having a bisphenol skeleton include an epoxy monomer having a bisphenol A type, bisphenol F type, or bisphenol S type bisphenol skeleton.

  Examples of the epoxy monomer having a dicyclopentadiene skeleton include dicyclopentadiene dioxide and a phenol novolac epoxy monomer having a dicyclopentadiene skeleton.

  Examples of the epoxy monomer having a naphthalene skeleton include 1-glycidylnaphthalene, 2-glycidylnaphthalene, 1,2-diglycidylnaphthalene, 1,5-diglycidylnaphthalene, 1,6-diglycidylnaphthalene, 1,7-diglycidyl. Naphthalene, 2,7-diglycidylnaphthalene, triglycidylnaphthalene, 1,2,5,6-tetraglycidylnaphthalene and the like can be mentioned.

  Examples of the epoxy monomer having an adamantane skeleton include 1,3-bis (4-glycidyloxyphenyl) adamantane and 2,2-bis (4-glycidyloxyphenyl) adamantane.

  Examples of the epoxy monomer having a fluorene skeleton include 9,9-bis (4-glycidyloxyphenyl) fluorene, 9,9-bis (4-glycidyloxy-3-methylphenyl) fluorene, and 9,9-bis (4- Glycidyloxy-3-chlorophenyl) fluorene, 9,9-bis (4-glycidyloxy-3-bromophenyl) fluorene, 9,9-bis (4-glycidyloxy-3-fluorophenyl) fluorene, 9,9-bis (4-Glycidyloxy-3-methoxyphenyl) fluorene, 9,9-bis (4-glycidyloxy-3,5-dimethylphenyl) fluorene, 9,9-bis (4-glycidyloxy-3,5-dichlorophenyl) Fluorene and 9,9-bis (4-glycidyloxy-3,5-dibromophenyl) Fluorene, and the like.

  Examples of the epoxy monomer having a biphenyl skeleton include 4,4'-diglycidylbiphenyl and 4,4'-diglycidyl-3,3 ', 5,5'-tetramethylbiphenyl.

  Examples of the epoxy monomer having a bi (glycidyloxyphenyl) methane skeleton include 1,1′-bi (2,7-glycidyloxynaphthyl) methane, 1,8′-bi (2,7-glycidyloxynaphthyl) methane, 1,1′-bi (3,7-glycidyloxynaphthyl) methane, 1,8′-bi (3,7-glycidyloxynaphthyl) methane, 1,1′-bi (3,5-glycidyloxynaphthyl) methane 1,8'-bi (3,5-glycidyloxynaphthyl) methane, 1,2'-bi (2,7-glycidyloxynaphthyl) methane, 1,2'-bi (3,7-glycidyloxynaphthyl) Examples include methane and 1,2′-bi (3,5-glycidyloxynaphthyl) methane.

  Examples of the epoxy monomer having a xanthene skeleton include 1,3,4,5,6,8-hexamethyl-2,7-bis-oxiranylmethoxy-9-phenyl-9H-xanthene.

  Specific examples of the oxetane compound (A1b) having an oxetanyl group include, for example, 4,4′-bis [(3-ethyl-3-oxetanyl) methoxymethyl] biphenyl, 1,4-benzenedicarboxylate bis [(3- Ethyl-3-oxetanyl) methyl] ester, 1,4-bis [(3-ethyl-3-oxetanyl) methoxymethyl] benzene, and oxetane-modified phenol novolac. As for an oxetane compound (A1b), only 1 type may be used and 2 or more types may be used together.

  From the viewpoint of further improving the heat resistance of the insulating layer that is a cured product, the curable compound (A) preferably has two or more cyclic ether groups.

  From the viewpoint of further improving the heat resistance of the cured product, the content of the curable compound having two or more cyclic ether groups in the total 100% by weight of the curable compound (A) is preferably 70% by weight or more. More preferably, it is 80% by weight or more and 100% by weight or less. The content of the curable compound having two or more cyclic ether groups in the total 100% by weight of the curable compound (A) may be 10% by weight or more and 100% by weight or less. Further, the entire curable compound (A) may be a curable compound having two or more cyclic ether groups.

  The molecular weight of the curable compound (A) is preferably less than 10,000. The molecular weight of the curable compound (A) is preferably 200 or more, more preferably 1200 or less, still more preferably 600 or less, and particularly preferably 550 or less. When the molecular weight of the curable compound (A) is not less than the above lower limit, the adhesiveness of the surface of the insulating layer is lowered, and the handleability of the laminate is further enhanced. When the molecular weight of the curable compound (A) is not more than the above upper limit, the adhesiveness of the cured product is further enhanced. Furthermore, the cured product is hard and hard to be brittle, and the adhesiveness of the cured product is further enhanced.

  In the present specification, the molecular weight in the curable compound (A) means a molecular weight that can be calculated from the structural formula when it is not a polymer and when the structural formula can be specified. Means weight average molecular weight.

  The curable compound (A) in a total of 100% by weight of the total resin components (hereinafter, may be abbreviated as the total resin component X) contained in the curable composition (the entire curable composition used for the insulating layer). ) Is preferably 50% by weight or more, more preferably 60% by weight or more, preferably 99.5% by weight or less, more preferably 99% by weight or less, and still more preferably 98% by weight or less. The content of the curable compound (A) is preferably 50% in a total of 100% by weight of the total resin components (hereinafter sometimes abbreviated as “total resin component X1”) contained in the first curable composition. % Or more, more preferably 60% by weight or more, preferably 99.5% by weight or less, more preferably 99% by weight or less, and still more preferably 98% by weight or less. The content of the curable compound (A) is preferably 50% in a total of 100% by weight of the total resin components (hereinafter sometimes abbreviated as “total resin component X2”) contained in the second curable composition. % Or more, more preferably 60% by weight or more, preferably 99.5% by weight or less, more preferably 99% by weight or less, and still more preferably 98% by weight or less. When the content of the curable compound (A) is not less than the above lower limit, the adhesiveness and heat resistance of the cured product are further enhanced. When the content of the curable compound (A) is not more than the above upper limit, the coating property of the curable composition is further enhanced. In addition, all the resin components X, X1, and X2 refer to the sum total of the curable compound (A), the curing agent (B), and other resin components added as necessary. The inorganic filler (C) is not included in all the resin components X, X1, and X2.

(Curing agent (B))
The insulating layer is preferably formed using a curing agent (B). Each of the first and second curable compositions preferably contains a curing agent (B). The curing agent (B) is not particularly limited as long as the curable composition can be cured. The curing agent (B) is preferably a thermosetting agent. As for the hardening | curing agent (B) used for an insulating layer, only 1 type may be used and 2 or more types may be used together. The curing agent (B) used for the first insulating layer and the curing agent (B) used for the second insulating layer may be the same or different.

  From the viewpoint of further improving the heat resistance of the cured product, the curing agent (B) preferably has an aromatic skeleton or an alicyclic skeleton. The curing agent (B) preferably includes an amine curing agent (amine compound), an imidazole curing agent, a phenol curing agent (phenol compound) or an acid anhydride curing agent (acid anhydride), and includes an amine curing agent. More preferred. The acid anhydride curing agent includes an acid anhydride having an aromatic skeleton, a water additive of the acid anhydride or a modified product of the acid anhydride, or an acid anhydride having an alicyclic skeleton, It is preferable to include a water additive of an acid anhydride or a modified product of the acid anhydride.

  From the viewpoint of improving the dispersibility of the inorganic filler (C) and further enhancing the voltage resistance and thermal conductivity of the cured product, the curing agent (B) preferably contains a basic curing agent. Further, from the viewpoint of further improving the dispersibility of the inorganic filler (C) and further increasing the voltage resistance and thermal conductivity of the cured product, the curing agent (B) is an amine curing agent or an imidazole curing agent. More preferably, it includes an amine curing agent, and particularly preferably includes dicyandiamide. Moreover, it is also preferable that a hardening | curing agent (B) contains both a dicyandiamide and an imidazole hardening | curing agent. By using these preferable curing agents, the dispersibility of the inorganic filler (C) in the curable composition is increased, and a cured product having an excellent balance of heat resistance, moisture resistance and electrical properties can be obtained. As a result, even if there is much content of an inorganic filler (C), thermal conductivity becomes quite high. In particular, when dicyandiamide is used, the adhesiveness between the cured product, the heat conductor, and the conductive layer is considerably increased.

  Examples of the amine curing agent include dicyandiamide, an imidazole compound, diaminodiphenylmethane, and diaminodiphenylsulfone. From the viewpoint of further enhancing the adhesion between the cured product, the heat conductor, and the conductive layer, the amine curing agent more preferably contains a dicyandiamide or an imidazole compound. From the viewpoint of further enhancing the storage stability of the insulating layer before curing, the curing agent (B) preferably contains a curing agent having a melting point of 180 ° C. or higher, and an amine curing agent having a melting point of 180 ° C. or higher. It is more preferable to contain.

  Examples of the imidazole curing agent include 2-undecylimidazole, 2-heptadecylimidazole, 2-methylimidazole, 2-ethyl-4-methylimidazole, 2-phenylimidazole, 2-phenyl-4-methylimidazole, and 1-benzyl. 2-methylimidazole, 1-benzyl-2-phenylimidazole, 1,2-dimethylimidazole, 1-cyanoethyl-2-methylimidazole, 1-cyanoethyl-2-ethyl-4-methylimidazole, 1-cyanoethyl-2- Undecylimidazole, 1-cyanoethyl-2-phenylimidazole, 1-cyanoethyl-2-undecylimidazolium trimellitate, 1-cyanoethyl-2-phenylimidazolium trimellitate, 2,4-diamino-6- [2 '-Methyl Midazolyl- (1 ′)]-ethyl-s-triazine, 2,4-diamino-6- [2′-undecylimidazolyl- (1 ′)]-ethyl-s-triazine, 2,4-diamino-6 [2′-Ethyl-4′-methylimidazolyl- (1 ′)]-ethyl-s-triazine, 2,4-diamino-6- [2′-methylimidazolyl- (1 ′)]-ethyl-s-triazine Isocyanuric acid adduct, 2-phenylimidazole isocyanuric acid adduct, 2-methylimidazole isocyanuric acid adduct, 2-phenyl-4,5-dihydroxymethylimidazole and 2-phenyl-4-methyl-5-dihydroxymethylimidazole Can be mentioned.

  Examples of the phenol curing agent include phenol novolak, o-cresol novolak, p-cresol novolak, t-butylphenol novolak, dicyclopentadiene cresol, polyparavinylphenol, bisphenol A type novolak, xylylene modified novolak, decalin modified novolak, poly ( And di-o-hydroxyphenyl) methane, poly (di-m-hydroxyphenyl) methane, and poly (di-p-hydroxyphenyl) methane. From the viewpoint of further enhancing the flexibility of the cured product and the flame retardancy of the cured product, a phenol resin having a melamine skeleton, a phenol resin having a triazine skeleton, or a phenol resin having an allyl group is preferable.

  Commercially available products of the phenol curing agent include MEH-8005, MEH-8010, and MEH-8015 (all of which are manufactured by Meiwa Kasei Co., Ltd.), YLH903 (manufactured by Mitsubishi Chemical Corporation), LA-7052, LA-7054, and LA-7751. LA-1356 and LA-3018-50P (all of which are manufactured by DIC Corporation), PS6313 and PS6492 (all of which are manufactured by Gunei Chemical Co., Ltd.), and the like.

  Examples of the acid anhydride having an aromatic skeleton, a water additive of the acid anhydride, or a modified product of the acid anhydride include, for example, a styrene / maleic anhydride copolymer, a benzophenone tetracarboxylic acid anhydride, and a pyromellitic acid anhydride. , Trimellitic anhydride, 4,4'-oxydiphthalic anhydride, phenylethynyl phthalic anhydride, glycerol bis (anhydrotrimellitate) monoacetate, ethylene glycol bis (anhydrotrimellitate), methyltetrahydroanhydride Examples include phthalic acid, methylhexahydrophthalic anhydride, and trialkyltetrahydrophthalic anhydride.

  Examples of commercially available acid anhydrides having an aromatic skeleton, water additives of the acid anhydrides, or modified products of the acid anhydrides include SMA Resin EF30, SMA Resin EF40, SMA Resin EF60, and SMA Resin EF80 (any of the above Also manufactured by Sartomer Japan), ODPA-M and PEPA (all manufactured by Manac), Ricacid MTA-10, Ricacid MTA-15, Ricacid TMTA, Ricacid TMEG-100, Ricacid TMEG-200, Ricacid TMEG-300, Ricacid TMEG-500, Ricacid TMEG-S, Ricacid TH, Ricacid HT-1A, Ricacid HH, Ricacid MH-700, Ricacid MT-500, Ricacid DSDA and Ricacid TDA-100 (all of which are manufactured by Shin Nippon Rika Co., Ltd.) PICLON B4400, EPICLON B650, and EPICLON B570 (all manufactured by both DIC Corporation).

  The acid anhydride having an alicyclic skeleton, a water additive of the acid anhydride, or a modified product of the acid anhydride is an acid anhydride having a polyalicyclic skeleton, a water additive of the acid anhydride, or the A modified product of an acid anhydride, or an acid anhydride having an alicyclic skeleton obtained by addition reaction of a terpene compound and maleic anhydride, a water additive of the acid anhydride, or a modified product of the acid anhydride It is preferable. By using these curing agents, the flexibility of the cured product and the moisture resistance and adhesion of the cured product are further increased.

  Examples of the acid anhydride having an alicyclic skeleton, a water addition of the acid anhydride, or a modified product of the acid anhydride include methyl nadic acid anhydride, acid anhydride having a dicyclopentadiene skeleton, and the acid anhydride And the like.

  Examples of commercially available acid anhydrides having the alicyclic skeleton, water additions of the acid anhydrides, or modified products of the acid anhydrides include Ricacid HNA and Ricacid HNA-100 (all of which are manufactured by Shin Nippon Rika Co., Ltd.) , And EpiCure YH306, EpiCure YH307, EpiCure YH308H, EpiCure YH309 (all of which are manufactured by Mitsubishi Chemical Corporation) and the like.

  The curing agent (B) is preferably methyl nadic acid anhydride or trialkyltetrahydrophthalic anhydride. Use of methyl nadic anhydride or trialkyltetrahydrophthalic anhydride increases the water resistance of the cured product.

  In the total 100% by weight of the total resin component X, the content of the curing agent (B) is preferably 0.5% by weight or more, more preferably 1% by weight or more, preferably 50% by weight or less, more preferably 40% by weight. % Or less. In the total 100% by weight of all the resin components X1, the content of the curing agent (B) is preferably 0.5% by weight or more, more preferably 1% by weight or more, preferably 50% by weight or less, more preferably 40% by weight. % Or less. The content of the curing agent (B) is preferably 0.5% by weight or more, more preferably 1% by weight or more, preferably 50% by weight or less, more preferably 40% by weight in the total 100% by weight of the total resin component X2. % Or less. It is easy to fully harden the whole curable composition as content of a hardening | curing agent (B) is more than the said minimum. When the content of the curing agent (B) is not more than the above upper limit, it is difficult to generate an excessive curing agent (B) that does not participate in curing. For this reason, the heat resistance and adhesiveness of hardened | cured material become still higher.

(Inorganic filler (C))
The insulating layer preferably contains an inorganic filler (C). The first and second insulating layers preferably include an inorganic filler having a thermal conductivity of 10 W / m · K or more. The curable composition preferably contains an inorganic filler (C). Each of the first and second curable compositions preferably contains an inorganic filler (C). The use of the inorganic filler (C) increases the thermal conductivity of the cured product. As a result, the thermal conductivity of the cured product is increased. As for the said inorganic filler (C), only 1 type may be used and 2 or more types may be used together. The inorganic filler (C) used for the first insulating layer and the inorganic filler (C) used for the second insulating layer may be the same or different.

  From the viewpoint of further increasing the thermal conductivity of the cured product, the thermal conductivity of the inorganic filler (C) is preferably 10 W / m · K or more, more preferably 15 W / m · K or more, and even more preferably 20 W / m. -K or more. The upper limit of the thermal conductivity of the inorganic filler (C) is not particularly limited. Inorganic fillers having a thermal conductivity of about 300 W / m · K are widely known, and inorganic fillers having a thermal conductivity of about 200 W / m · K are easily available.

  The inorganic filler (C) is preferably at least one selected from the group consisting of alumina, synthetic magnesite, crystalline silica, boron nitride, aluminum nitride, silicon nitride, silicon carbide, zinc oxide and magnesium oxide, More preferably, it is at least one selected from the group consisting of alumina, crystalline silica, boron nitride and aluminum nitride. Use of these preferable inorganic fillers further increases the thermal conductivity of the cured product.

  The inorganic filler (C) is more preferably at least one selected from the group consisting of spherical alumina, crushed alumina, crystalline silica, boron nitride, aggregated particles, and spherical aluminum nitride. Use of these preferable fillers further increases the thermal conductivity of the cured product. The boron nitride and the aggregated particles are preferably boron nitride and boron nitride aggregated particles that are not aggregated particles.

  The inorganic filler (C) preferably contains an inorganic filler having a new Mohs hardness of 12 or less. The new Mohs hardness of the inorganic filler having the new Mohs hardness of 12 or less is more preferably 9 or less. Use of an inorganic filler having a new Mohs hardness of not more than the above upper limit further increases the workability of the cured product.

  From the viewpoint of further improving the workability of the cured product, the inorganic filler (C) is preferably at least one selected from the group consisting of synthetic magnesite, crystalline silica, zinc oxide, and magnesium oxide. The new Mohs hardness of these inorganic fillers is 9 or less.

  The inorganic filler (C) may contain a spherical filler (spherical filler), may contain a crushed filler (crushed filler), or may contain a plate-like filler (plate-like filler). Good. It is particularly preferable that the inorganic filler (C) includes a spherical filler. Since spherical fillers can be filled at high density, the use of spherical fillers further increases the thermal conductivity of the cured product.

  Examples of the crushed filler include crushed alumina. The crushing filler is obtained, for example, by crushing a lump-like inorganic substance using a uniaxial crusher, a biaxial crusher, a hammer crusher, a ball mill, or the like. By using the crushed filler, the filler in the insulating layer tends to be bridged or have a structure in which the filler is effectively brought into close proximity. Therefore, the thermal conductivity of the cured product is further increased. Moreover, generally the crushing filler is cheap compared with a normal filler. For this reason, the cost of a laminated body becomes low by use of a crushing filler.

  The average particle diameter of the crushed filler is preferably 12 μm or less, more preferably 10 μm or less, and preferably 1 μm or more. When the average particle size of the crushed filler is not more than the above upper limit, the crushed filler can be dispersed with high density in the curable composition, and the withstand voltage of the cured product is further enhanced. When the average particle diameter of the crushed filler is not less than the above lower limit, it becomes easy to fill the crushed filler with high density.

  The aspect ratio of the crushing filler is not particularly limited. The aspect ratio of the crushed filler is preferably 1.5 or more, and preferably 20 or less. Fillers with an aspect ratio of less than 1.5 are relatively expensive and increase the cost of the laminate. When the aspect ratio is 20 or less, filling of the crushed filler is easy.

  The aspect ratio of the crushed filler can be determined, for example, by measuring the crushed surface of the filler using a digital image analysis particle size distribution measuring apparatus (“FPA” manufactured by Nippon Luft).

  When the inorganic filler (C) is a spherical filler, the average particle diameter of the spherical filler is preferably 0.1 μm or more, and preferably 40 μm or less. When the average particle size is 0.1 μm or more, the inorganic filler (C) can be easily filled at a high density. When the average particle size is 40 μm or less, the voltage resistance of the cured product is further enhanced.

  The “average particle diameter” is an average particle diameter obtained from a volume average particle size distribution measurement result measured by a laser diffraction particle size distribution measuring apparatus.

  From the viewpoint of suppressing thickness variation of the cured product and effectively increasing the thermal conductivity of the cured product, the maximum particle size of the inorganic filler (C) is preferably 70 μm or less, more preferably 50 μm or less. In addition, the maximum particle diameter of the said crushing filler and the said plate-shaped filler means the major axis of the largest particle.

  The content of the inorganic filler (C) in 100% by weight of the insulating layer is preferably 70% by weight or more, more preferably 75% by weight or more, still more preferably 80% by weight or more, particularly preferably 85% by weight or more, and most preferably 86 wt% or more, preferably less than 97 wt%, more preferably less than 95 wt%. In 100% by weight of the curable composition (the whole curable composition used for the insulating layer), the content of the inorganic filler (C) is 70% by weight or more, more preferably 75% by weight or more, and further preferably 80% by weight or more. Particularly preferably, it is 85% by weight or more, most preferably 86% by weight or more, preferably less than 97% by weight, more preferably less than 95% by weight. When the content of the inorganic filler (C) in the insulating layer and the curable composition is not less than the above lower limit and not more than the above upper limit, the cured state of the insulating layer, which is a cured product, becomes good and the thermal conductivity becomes considerably high. .

  In 100% by weight of the first insulating layer and in 100% by weight of the first curable composition, the content of the inorganic filler (C) is 70% by weight or more, more preferably 75% by weight or more, and still more preferably 80% by weight. Above, particularly preferably 85% by weight or more, most preferably 86% by weight or more, preferably less than 97% by weight, more preferably less than 95% by weight. When the content of the inorganic filler (C) in the first insulating layer and the first curable composition is not less than the above lower limit and not more than the above upper limit, the cured state of the first insulating layer that is a cured product is favorable. And the thermal conductivity is considerably high.

  In 100% by weight of the second insulating layer and 100% by weight of the second curable composition, the content of the inorganic filler (C) is preferably 67% by weight or more, preferably less than 97% by weight, more preferably 95% by weight. %. When the content of the inorganic filler (C) in the second insulating layer and the second curable composition is not less than the above lower limit and not more than the above upper limit, the cured state of the second insulating layer that is a cured product is favorable. And the adhesion between the second insulating layer, which is a cured product, and the conductive layer is considerably increased.

  From the viewpoint of improving both the thermal conductivity of the entire insulating layer and the adhesion between the second insulating layer, which is a cured product, and the conductive layer in a well-balanced manner, the insulation located on the surface of the insulating layer on the copper plate side The content of the inorganic filler in the layer portion is preferably larger than the content of the inorganic filler in the insulating layer portion located on the surface opposite to the copper plate side of the insulating layer, more preferably 1% by weight or more. More preferably 5% by weight or more, and more preferably 10% by weight or more. From the viewpoint of improving both the thermal conductivity of the entire insulating layer and the adhesion between the second insulating layer, which is a cured product, and the conductive layer in a balanced manner, an inorganic filler (100 wt% of the first insulating layer) The content of C) is preferably greater than the content of the inorganic filler (C) in 100% by weight of the second insulating layer, more preferably 1% by weight or more, and more preferably 5% by weight or more. Preferably, it is more than 10% by weight.

  From the viewpoint of improving both the thermal conductivity of the entire insulating layer and the adhesion between the second insulating layer, which is a cured product, and the conductive layer in a well-balanced manner, an inorganic filler (100% by weight of the second insulating layer) Ratio of content of C) to content of inorganic filler (C) in 100% by weight of first insulating layer (content of inorganic filler (C) in 100% by weight of second insulating layer / first The content of the inorganic filler (C) in 100% by weight of the insulating layer) is preferably 0.7 or more, and preferably 0.95 or less.

(Other ingredients)
The insulating layer and the curable composition may include a polymer having a weight average molecular weight of 10,000 or more. As for this polymer, only 1 type may be used and 2 or more types may be used together.

  As the polymer, a curable resin such as a thermoplastic resin and a thermosetting resin can be used. The polymer is preferably a curable resin.

  The thermoplastic resin and thermosetting resin are not particularly limited. The thermoplastic resin is not particularly limited, and examples thereof include styrene resin, phenoxy resin, phthalate resin, thermoplastic urethane resin, polyamide resin, thermoplastic polyimide resin, ketone resin, and norbornene resin. The thermosetting resin is not particularly limited, and examples thereof include amino resins, phenol resins, thermosetting urethane resins, epoxy resins, thermosetting polyimide resins, and amino alkyd resins. Examples of the amino resin include urea resin and melamine resin.

  From the viewpoint of suppressing the oxidative degradation of the cured product, further improving the heat cycle resistance and heat resistance of the cured product, and further reducing the water absorption rate of the cured product, the polymer is a styrene resin, phenoxy resin or epoxy resin. It is preferable that it is a phenoxy resin or an epoxy resin, more preferably a phenoxy resin. In particular, use of a phenoxy resin or an epoxy resin further increases the heat resistance of the cured product. Moreover, use of a phenoxy resin further lowers the elastic modulus of the cured product and further improves the cold-heat cycle characteristics of the cured product. The polymer may not have a cyclic ether group such as an epoxy group.

  As the styrene resin, specifically, a homopolymer of a styrene monomer, a copolymer of a styrene monomer and an acrylic monomer, or the like can be used. Among these, a styrene polymer having a styrene-glycidyl methacrylate structure is preferable.

  Examples of the styrene monomer include styrene, o-methylstyrene, m-methylstyrene, p-methylstyrene, p-methoxystyrene, p-phenylstyrene, p-chlorostyrene, p-ethylstyrene, and pn-. Butyl styrene, p-tert-butyl styrene, pn-hexyl styrene, pn-octyl styrene, pn-nonyl styrene, pn-decyl styrene, pn-dodecyl styrene, 2,4-dimethyl Examples include styrene and 3,4-dichlorostyrene.

  Specifically, the phenoxy resin is, for example, a resin obtained by reacting an epihalohydrin with a divalent phenol compound, or a resin obtained by reacting a divalent epoxy compound with a divalent phenol compound.

  The phenoxy resin comprises a bisphenol A skeleton, a bisphenol F skeleton, a bisphenol A / F mixed skeleton, a naphthalene skeleton, a fluorene skeleton, a biphenyl skeleton, an anthracene skeleton, a pyrene skeleton, a xanthene skeleton, an adamantane skeleton, and a dicyclopentadiene skeleton. It is preferred to have at least one skeleton selected from the group. Among these, the phenoxy resin preferably has at least one skeleton selected from the group consisting of a bisphenol A skeleton, a bisphenol F skeleton, a bisphenol A / F mixed skeleton, a naphthalene skeleton, a fluorene skeleton, and a biphenyl skeleton. Preferably, it has at least one skeleton of a fluorene skeleton and a biphenyl skeleton. Use of the phenoxy resin having these preferable skeletons further increases the heat resistance of the cured product.

  The epoxy resin is an epoxy resin other than the phenoxy resin. Examples of the epoxy resins include styrene skeleton-containing epoxy resins, bisphenol A type epoxy resins, bisphenol F type epoxy resins, bisphenol S type epoxy resins, phenol novolac type epoxy resins, biphenol type epoxy resins, naphthalene type epoxy resins, and fluorene type epoxy resins. , Phenol aralkyl type epoxy resin, naphthol aralkyl type epoxy resin, dicyclopentadiene type epoxy resin, anthracene type epoxy resin, epoxy resin having adamantane skeleton, epoxy resin having tricyclodecane skeleton, and epoxy resin having triazine nucleus in skeleton Etc.

  In the total 100% by weight of the total resin component X, in the total 100% by weight of the total resin component X1, and in the total 100% by weight of the total resin component X2, the content of the polymer is preferably 20% by weight. Above, more preferably 30% by weight or more, preferably 60% by weight or less, more preferably 50% by weight or less. When the content of the polymer is not less than the above lower limit, the handleability of the curable composition is improved. When the polymer content is not more than the above upper limit, dispersion of the inorganic filler (C) becomes easy. The all resin components X, X1, and X2 include a polymer.

  The insulating layer and the curable composition may contain rubber particles. Use of the rubber particles increases the stress relaxation property and flexibility of the cured product. The insulating layer and the curable composition may contain a dispersant. Use of the dispersant further increases the thermal conductivity and voltage resistance of the cured product.

  The insulating layer and the curable composition may contain a base material such as glass cloth, glass nonwoven fabric, and aramid nonwoven fabric. The insulating layer and the curable composition preferably do not contain a base material, and particularly preferably do not contain glass cloth. When the insulating layer and the curable composition do not contain the base material, the thickness of the entire insulating layer is reduced, and the thermal conductivity of the cured product is further increased. Various processing such as laser processing or drilling can be easily performed. The insulating layer may not be a prepreg.

  Furthermore, the insulating layer and the curable composition may be a silane coupling agent, an antioxidant, an ion scavenger, a tackifier, a plasticizer, a thixotropic agent, a photosensitizer, and a color as necessary. An agent or the like may be included. The all resin components X, X1, and X2 contain a silane coupling agent.

(Details of laminate)
The manufacturing method of the said laminated body is not specifically limited. As this manufacturing method, for example, after coating the curable composition on a heat conductor by a solvent cast method or the like, and proceeding with the curing of the curable composition as necessary to form an insulating layer , A method of laminating a protective film on the insulating layer, and after the curable composition is coated on the release film by a solvent casting method or the like to form the curable composition sheet, the curing is performed on the heat conductor And a method of laminating a curable composition sheet, then proceeding with curing of the curable composition as necessary to form an insulating layer, and laminating a protective film on the insulating layer. Curing of the curable composition may be performed before the insulating layer is laminated on the heat conductor, may be performed after the insulating layer is laminated, or may be performed before the protective film is laminated on the insulating layer. It may be performed after being laminated. Moreover, the manufacturing method of the said laminated body is not limited to this method.

  In addition, when the insulating layer is a multilayer, the method for manufacturing the laminate is not particularly limited. As this manufacturing method, for example, the above-described curable composition is applied on a heat conductor by a solvent casting method or the like, and the first curable composition is cured to form a first insulating layer. Then, the second curable composition described above is applied onto the first insulating layer by a solvent casting method or the like, and the curing of the second curable composition is advanced as necessary. After forming the insulating layer 2, the method for laminating the protective film on the insulating layer, and the above-mentioned curable composition by applying the first curable composition described above on the release film by a solvent casting method or the like After forming the product sheet, laminating the curable composition sheet on the heat conductor, and then, if necessary, proceeding with the curing of the first curable composition to form the first insulating layer, A second curable composition sheet formed in the same manner is laminated on the first insulating layer, and as necessary. After forming the second second insulating layer is allowed to proceed the curing of the curable composition of Te, and a method of laminating a protective film on the insulating layer. Moreover, hardening of a 1st curable composition may be performed after the lamination and application | coating of a 2nd curable composition. Curing of the first curable composition may be performed before or after the first insulating layer is laminated on the thermal conductor. In addition, the first and second insulating layers may be formed by an extrusion method. Moreover, the manufacturing method of the said laminated body is not limited to these methods.

  The thermal conductivity of the insulating layer (the entire insulating layer) is preferably 2 W / m · K or more, more preferably 3 W / m · K or more, still more preferably 4 W / m · K or more, and particularly preferably 5 W / m · K. That's it. The higher the thermal conductivity of the insulating layer, the higher the thermal conductivity of the entire insulating layer.

  The dielectric breakdown voltage of the cured insulating layer (the entire insulating layer) is preferably 30 kV or higher, more preferably 40 kV or higher, still more preferably 50 kV or higher, particularly preferably 80 kV or higher, and most preferably 100 kV or higher. The higher the dielectric breakdown voltage, the more sufficient insulation can be ensured when the laminate is used for large current applications such as for power devices.

  In FIG. 1, an example of the laminated body which concerns on one Embodiment of this invention is shown with sectional drawing.

  The laminate 1 shown in FIG. 1 includes a heat conductor 2 having a thermal conductivity of 10 W / m · K or more, an insulating layer 3, and a protective film layer 4. The insulating layer 3 includes a first insulating layer 3A and a second insulating layer 3B. The protective film layer 4 has the base material 4A and the adhesion part 4B.

  The insulating layer 3 is laminated on the surface of the heat conductor 2. The first insulating layer 3 </ b> A is laminated on the surface of the heat conductor 2. The second insulating layer 3B is laminated on the surface opposite to the heat conductor 2 side of the first insulating layer 3A. The protective film layer 4 is laminated on the surface opposite to the heat conductor 2 side of the insulating layer 3. The protective film layer 4 is laminated on the surface of the second insulating layer 3B opposite to the first insulating layer 3A side. The adhesive portion 4B is laminated on the surface of the insulating layer 3 opposite to the heat conductor 2 side. 4 A of base materials are laminated | stacked on the surface on the opposite side to the insulating layer 3 side of the adhesion part 4B.

  FIG. 2 is a cross-sectional view showing an example of a power semiconductor module component obtained using the laminate according to one embodiment of the present invention.

  A power semiconductor module component 11 shown in FIG. 2 is formed using the above-described laminate 1. However, the insulating layer 3 in the laminate 1 is cured. Moreover, the protective film layer 4 is peeled from the surface of the insulating layer 3 when the laminate 1 is used, and the power semiconductor module component 11 does not have the protective film layer 4.

  The power semiconductor module component 11 includes a heat conductor 2 having a thermal conductivity of 10 W / m · K or more, an insulating layer 3 that is a cured product, a conductive layer 12, and a mold resin 13. The insulating layer 3 that is a cured product includes a first insulating layer 3A that is a cured product, and a second insulating layer 3B that is a cured product.

  The conductive layer 12 is laminated on the surface of the insulating layer 3 opposite to the heat conductor 2 side. The conductive layer 12 is laminated on the surface of the second insulating layer 3B opposite to the first insulating layer 3A side. The heat conductor 2, the insulating layer 3, and the conductive layer 12 are embedded in the mold resin 13. Part of the conductive layer 12 is preferably exposed from the mold resin 13.

  In the power semiconductor module component 11, the protective film layer 4 is peeled off from the surface of the insulating layer 3 in the laminate 1, the conductive layer 12 is laminated on the exposed surface of the insulating layer 3, and then the insulating layer 3 is cured. Further, it is obtained by embedding the heat conductor 2, the insulating layer 3, and the conductive layer 12 in the mold resin 13. At this time, it is preferable that the thermal conductor 2, the insulating layer 3, and the conductive layer 12 are embedded in the mold resin 13 so that a part of the conductive layer 12 is exposed. Alternatively, the insulating layer 3 may be cured after the thermal conductor 2, the insulating layer 3, and the conductive layer 12 are embedded in the mold resin 13. For example, the insulating layer 3 may be cured when the mold resin 13 is cured.

  Moreover, the use of the laminate is not limited to the power semiconductor module component described above. Using the above laminated body, for example, a metal body is bonded to each conductive layer such as a laminated board or a multilayer wiring board provided with copper circuits on both sides, a copper foil, a copper plate, a semiconductor element or a semiconductor package via an insulating layer. Various electric parts that are used may be obtained. The laminate is suitably used for adhering a heat conductor to a conductive layer of a semiconductor device in which a semiconductor element is mounted on a substrate. Furthermore, the laminated body adheres a thermal conductor having a thermal conductivity of 10 W / m · K or more to a conductive layer of an electronic component device in which electronic component elements other than semiconductor elements are mounted on a substrate. Are also preferably used.

  The heat conductor whose heat conductivity is 10 W / m · K or more is not particularly limited. Examples of the heat conductor having a thermal conductivity of 10 W / m · K or more include aluminum, copper, alumina, beryllia, silicon carbide, silicon nitride, aluminum nitride, and graphite sheet. Especially, it is preferable that the heat conductor whose said heat conductivity is 10 W / m * K or more is copper or aluminum. Copper or aluminum is excellent in heat dissipation.

  Hereinafter, the present invention will be clarified by giving specific examples and comparative examples of the present invention. The present invention is not limited to the following examples.

  In order to form the insulating layer, the following materials were prepared.

[polymer]
(1) Bisphenol A type phenoxy resin (“E1256” manufactured by Mitsubishi Chemical Corporation, Mw = 51000)
(2) Polystyrene (“HRM26” manufactured by Toyo Styrene Co., Ltd., Mw = 300,000)

[Curable compound (A)]
(1) Bisphenol A liquid epoxy resin ("Epicoat 828US" manufactured by Mitsubishi Chemical Corporation, Mw = 370)
(2) Bisphenol F type liquid epoxy resin (“Epicoat 806L” manufactured by Mitsubishi Chemical Corporation, Mw = 370)
(3) Naphthalene skeleton liquid epoxy resin (“EPICLON HP-4032D” manufactured by DIC, Mw = 304)
(4) Biphenyl skeleton epoxy resin (“Epicoat YX4000” manufactured by Mitsubishi Chemical Corporation, Mw = 368)

[Curing agent (B)]
(1) Alicyclic skeleton acid anhydride (“MH-700” manufactured by Shin Nippon Rika Co., Ltd.)
(2) Biphenyl skeleton phenolic resin (“MEH-7851-S” manufactured by Meiwa Kasei Co., Ltd.)
(3) Diaminodiphenylmethane (melting point 90 ° C)
(4) Dicyandiamide (melting point 208 ° C)
(5) Isocyanur-modified solid dispersion type imidazole (“2MZA-PW” manufactured by Shikoku Kasei Co., Ltd., melting point 253 ° C.)

[Inorganic filler (C)]
(1) 5 μm crushed alumina (crushed filler, “LT300C” manufactured by Nippon Light Metal Co., Ltd., average particle diameter 5 μm, maximum particle diameter 15 μm, thermal conductivity 36 W / m · K, new Mohs hardness 12)
(2) Spherical alumina (“DAM-10” manufactured by Denka Co., Ltd., average particle size 10 μm, maximum particle size 30 μm, thermal conductivity 36 W / m · K, new Mohs hardness 12)
(3) Aluminum nitride (“TOYALNITE-FLX” manufactured by Toyo Aluminum Co., Ltd., average particle size 14 μm, maximum particle size 30 μm, thermal conductivity 200 W / m · K, new Mohs hardness 11)
(4) Crystalline silica (“Crystallite CMC-12” manufactured by Tatsumori Co., Ltd., average particle size 5 μm, maximum particle size 20 μm, thermal conductivity 10 W / m · K, new Mohs hardness 9)
(5) Boron nitride agglomerated particles (“TPX25” manufactured by Momentive, average particle diameter 25 μm, maximum particle diameter 100 μm, thermal conductivity 60 W / m · K, new Mohs hardness 2)
(6) Fused silica (“SE15” manufactured by Tokuyama Corporation, average particle size 15 μm, maximum particle size 60 μm, thermal conductivity 2 W / m · K, new Mohs hardness 7)

[Additive]
(1) Epoxysilane coupling agent (“KBE403” manufactured by Shin-Etsu Chemical Co., Ltd.)

[solvent]
(1) Methyl ethyl ketone In order to form a protective film layer, the following protective films were prepared.

[Protective film having uneven surface]
(1) Type 1: Protective film 1 (Both surfaces of the base material and the adhesive part have an uneven shape by embossing, thickness 50 μm, base material: PET, ten-point average roughness Rz of 5 μm of the adhesive part)
(2) Type 2: Protective film 2 (The surface of the substrate does not have an uneven shape, the surface of the adhesive portion has an uneven shape by embossing, the thickness of the protective film is 50 μm, the thickness of the adhesive portion is 30 μm, the substrate: PET, ten point average roughness of adhesive part Rz 30 μm)
(3) Type 3: Protective film 3 (The surface of the substrate does not have an uneven shape, the surface of the adhesive portion has an uneven shape by embossing, the thickness of the protective film is 40 μm, the thickness of the adhesive portion is 30 μm, the substrate: PET, ten point average roughness of adhesive part Rz 30 μm)
(4) Type 4: Protective film 4 (The surface of the substrate does not have an uneven shape, the surface of the adhesive portion has an uneven shape by embossing, the thickness of the protective film is 80 μm, the thickness of the adhesive portion is 40 μm, the substrate: PET, ten point average roughness of adhesive part Rz 30 μm)
(5) Type 5: Protective film 5 (the surface of the substrate does not have an uneven shape, the surface of the adhesive portion has an uneven shape by embossing, the thickness of the protective film is 150 μm, the thickness of the adhesive portion is 40 μm, the substrate: PET, ten point average roughness of adhesive part Rz 30 μm)
(6) Type 6: protective film 6 (the surface of the substrate does not have an uneven shape, the surface of the adhesive portion has an uneven shape by embossing, the thickness of the protective film is 180 μm, the thickness of the adhesive portion is 40 μm, the substrate: PET, ten point average roughness of adhesive part Rz 30 μm)
(7) Type 7: Protective film 7 (the surface of the substrate does not have an uneven shape, the surface of the adhesive portion has an uneven shape by embossing, the thickness of the protective film is 180 μm, the thickness of the adhesive portion is 80 μm, the substrate: PET, ten point average roughness of adhesive part Rz60μm)
(8) Type 8: Protective film 8 (the surface of the substrate does not have an uneven shape, the surface of the adhesive portion has an uneven shape by embossing, the thickness of the protective film is 80 μm, the thickness of the adhesive portion is 60 μm, the substrate: PET, ten point average roughness of adhesive part Rz 50 μm)
(9) Type 9: Protective film 9 (the surface of the substrate does not have an uneven shape, the surface of the adhesive portion has an uneven shape by embossing, the thickness of the protective film is 50 μm, the thickness of the adhesive portion is 10 μm, the substrate: PET, ten-point average roughness of adhesive part Rz 10 μm)
(10) Type 10: protective film 10 (the surface of the substrate does not have an uneven shape, the surface of the adhesive portion has an uneven shape by embossing, the thickness of the protective film is 20 μm, the thickness of the adhesive portion is 3 μm, the substrate: PET, ten point average roughness of adhesive part Rz3μm)
(11) Type 11: Protective film 11 (the surface of the substrate does not have an uneven shape, the surface of the adhesive portion has an uneven shape by embossing, the thickness of the protective film is 20 μm, the thickness of the adhesive portion is 1 μm, the substrate: PET, ten-point average roughness of adhesive part Rz 0.5 μm)
(12) Type 12: Protective film 12 (the surface of the substrate does not have an uneven shape, the surface of the adhesive portion has an uneven shape by embossing, the thickness of the protective film is 15 μm, the thickness of the adhesive portion is 3 μm, the substrate: PET, ten point average roughness of adhesive part Rz3μm)
(13) Type 13: Protective film 13 (the surface of the substrate does not have an uneven shape, the surface of the adhesive portion has an uneven shape by embossing, the thickness of the protective film is 50 μm, the thickness of the adhesive portion is 3 μm, the substrate: PE, ten point average roughness of adhesive part Rz3μm)

[Protective film that does not have uneven surface]
(1) Type A: Protective film A (having a base material and an adhesive part, both surfaces of the base material and the adhesive part are not uneven, the thickness of the protective film is 50 μm, the thickness of the adhesive part is 30 μm, the base material: PET)
(2) Type B: Protective film B (non-adhesive base material only, no adhesive part, base material surface does not have uneven shape, protective film thickness 50 μm, base material: PET)

Example 1
A first curable composition for forming a first insulating layer, using a homodisper type stirrer, blending and kneading each component in the proportions shown in Table 1 below (the blending unit is parts by weight), and A second curable composition for forming a second insulating layer was prepared.

  The first curable composition was applied onto a release PET sheet having a thickness of 50 μm and dried in an oven at 90 ° C. for 30 minutes to produce a first insulating layer having a thickness of 80 μm on the PET sheet. In addition, the second curable composition was coated on a release PET sheet having a thickness of 50 μm and dried in an oven at 90 ° C. for 30 minutes to produce a second insulating layer having a thickness of 80 μm on the PET sheet. .

  The obtained first insulating layer was bonded to a copper plate (Cu) having a thickness of 0.5 mm using a thermal laminator and then cured at 200 ° C. for 1 hour (curing conditions for the first curable composition). . Thereafter, the second insulating layer was bonded onto the first insulating layer using a thermal laminator and then cured at 130 ° C. for 3 minutes (curing conditions for the second curable composition). Next, a protective film was applied to the surface of the second insulating layer from the pressure-sensitive adhesive side by reciprocating a 2 kg rubber roller at 25 ° C. once to form a protective film layer, thereby producing a laminate.

(Examples 2 to 30)
Table 1 below shows the types and amounts of the components used in the first and second curable compositions, the curing conditions of the second curable composition, and the types of protective films used in obtaining the laminate. A curable composition was prepared in the same manner as in Example 1 except that it was shown in -4 to obtain a laminate.

(Comparative Example 1)
A laminate was obtained in the same manner as in Example 1 except that the protective film was changed to the protective film A.

(Comparative Example 2)
A laminate was obtained in the same manner as in Example 1 except that the protective film was changed to the protective film B.

(Comparative Example 3)
A copper plate having a thickness of 0.5 mm was changed to an FR-4 substrate (FR-4) having a thickness of 0.5 μm, and the protective film was changed to a protective film B in the same manner as in Example 1, A laminate was obtained.

(Evaluation)
(1) Peelability of protective film layer The obtained laminate was cut by press punching into a size of 1 cm x 5 cm with a 45 ton press to obtain an evaluation sample. An adhesive tape (“CT24” manufactured by Nichiban) was attached to the protective film layer of the obtained evaluation sample by reciprocating a 2 kg rubber roller once at 25 ° C., and then the protective film layer was peeled off from the surface of the insulating layer. The peelability of the protective film layer was determined according to the following criteria.

[Peelability of protective film layer]
○: No peeling failure in all 20 evaluation samples ○: 1-2 occurrences of peeling failure in 20 evaluation samples Δ: 3-4 occurrences of peeling failure in 20 evaluation samples X: Out of 20 evaluation samples, 5 or more occurrences of peeling failure occurred

(2) Adhesive change before and after press punching The obtained laminate was cut by press punching into a size of 5 cm × 5 cm with a 45 ton press to obtain an evaluation sample. The peel strength after punching of the protective film layer and the insulating layer in the obtained evaluation sample was measured by a 90 ° peel test.

  Separately, a laminate without a protective film was prepared and cut into a size of 5 cm × 5 cm without performing pressing. Thereafter, a protective film was applied to the surface of the second insulating layer by reciprocating a 2 kg rubber roller once at 25 ° C. to form a protective film layer, and an evaluation sample was prepared. The peel strength before punching of the protective film layer and the insulating layer in the obtained evaluation sample was measured by a 90 ° peel test. Changes in adhesion before and after press punching were judged according to the following criteria.

[Criteria for adhesive change before and after punching]
○: The peel strength after punching is less than 130% of the peel strength before punching Δ: The peel strength after punching is 130% or more and less than 200% of the peel strength before punching ×: The peel strength after punching Is 200% or more of the peel strength before punching

(3) Dielectric breakdown voltage (withstand voltage)
The obtained laminate was cut into a size of 5 cm × 5 cm by press punching with a 45 ton press. Thereafter, an insulating layer having a size of 5 cm × 5 cm (entire insulating layer) was taken out to obtain an evaluation sample. The obtained evaluation sample was cured in an oven at 200 ° C. for 1 hour to obtain an insulating layer as a cured product. Using a withstand voltage tester (“MODEL7473” manufactured by EXTECH Electronics), an AC voltage was applied between the insulating layers so that the voltage increased at a rate of 1 kV / sec. The voltage at which the insulating layer was broken was taken as the breakdown voltage. The dielectric breakdown voltage was evaluated for 100 insulating layers, and the average value was obtained.

(4) Stability of dielectric breakdown voltage (voltage resistance) From the evaluation result of (3) dielectric breakdown voltage (voltage resistance), the stability of dielectric breakdown voltage was determined according to the following criteria.

[Stability of dielectric breakdown voltage (voltage resistance)]
O: The number of insulating layers whose dielectric breakdown voltage is 3 kV or more lower than the average value of the dielectric breakdown voltages of 100 insulating layers is 0 to 1 Δ: The average value of the dielectric breakdown voltages of 100 insulating layers is Number of insulating layers whose dielectric breakdown voltage is 3 kV or more is 2 to 4 ×: The number of insulating layers whose dielectric breakdown voltage is 3 kV or more lower than the average value of the dielectric breakdown voltages of 100 insulating layers is 5 or more

(5) Heat dissipation The obtained laminate was cut into a size of 5 cm × 5 cm by press punching with a 45 ton press to obtain an evaluation sample. Using the obtained evaluation sample, the protective film was peeled off from the surface of the insulating layer, and the exposed surface of the insulating layer was applied to a smooth heating element controlled to 60 ° C. of the same size at a pressure of 196 N / cm ² . Pressed with. The surface temperature of the copper plate was measured by a thermocouple. The heat dissipation was determined according to the following criteria.

[Criteria for heat dissipation]
○: Temperature difference between the heating element and the surface of the copper plate exceeds 3 ° C. and within 6 ° C. Δ: Temperature difference between the heating element and the surface of the copper plate exceeds 6 ° C. and within 10 ° C. ×: Temperature of the heating element on the surface of the copper plate The difference exceeds 10 ° C

(6) Adhesiveness The obtained laminate was cut into a size of 5 cm × 5 cm by press punching with a 45 ton press to obtain an evaluation sample. Using the obtained evaluation sample, the protective film was peeled off from the surface of the insulating layer, and heated at 200 ° C. for 1 hour while pressing an electrolytic copper foil having a thickness of 35 μm on the exposed surface of the insulating layer with a pressure of 1 MPa. . Thereafter, the peel strength between the insulating layer, which is a cured product, and the copper foil was measured by a 90 ° peel test.

  The blending components and results are shown in Tables 1 to 4 below.

DESCRIPTION OF SYMBOLS 1 ... Laminated body 2 ... Thermal conductor 3 ... Insulating layer 3A ... 1st insulating layer 3B ... 2nd insulating layer 4 ... Protective film layer 4A ... Base material 4B ... Adhesive part 11 ... Power semiconductor module component 12 ... Conductivity Layer 13 ... Mold resin

Claims (12)

A thermal conductor having a thermal conductivity of 10 W / m · K or more;
An insulating layer laminated on the surface of the thermal conductor;
A protective film layer laminated on the surface opposite to the heat conductor side of the insulating layer,
The protective film layer has a base material and an adhesive part laminated on the surface of the base material, and the protective film layer is laminated on the surface of the insulating layer from the adhesive part side,
The laminate, wherein the protective film layer has a concavo-convex shape on the surface of the adhesive portion on the insulating layer side.   The laminate according to claim 1, wherein a surface of the adhesive portion on the insulating layer side is embossed.   The laminate according to claim 1 or 2, wherein the protective film layer does not have a concavo-convex shape on a surface opposite to the adhesive portion side of the base material.   The laminated body of any one of Claims 1-3 whose ratio with respect to the thickness of the said insulating layer of the thickness of the said protective film layer is 0.2 or more and 1 or less.   The laminate according to any one of claims 1 to 4, wherein a ten-point average roughness Rz of the surface of the adhesive portion on the insulating layer side is 1 µm or more and 50 µm or less.   The laminate according to any one of claims 1 to 5, wherein the protective film layer is colored.   The laminated body of any one of Claims 1-6 in which the said insulating layer contains the inorganic filler whose heat conductivity is 10 W / m * K or more.   The laminate according to any one of claims 1 to 7, wherein the insulating layer has a plurality of layers having different curing rates and is a multilayer.   The laminated body of any one of Claims 1-8 whose hardening rate of the surface at the side of the said protective film layer of the said insulating layer is 20% or more and 80% or less.   The laminate according to any one of claims 1 to 9, wherein a material of the base material is a polyester resin.   The cutting laminated body obtained by cut | disconnecting the laminated body of any one of Claims 1-10 in the state in which the said heat conductor, the said insulating layer, and the said protective film layer were laminated | stacked.   The cut laminated body according to claim 11, which is obtained by cutting the laminated body by press punching.

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