Resin composition and syringe filled with resin composition

Abstract

This invention provides a syringe filled with a resin composition that has good distribution, dispensing performance, and resin flowability. The syringe of this invention comprises a syringe and a resin composition filled within the syringe. The resin composition is distributed on the surface of a horizontally positioned silicon wafer to form a resin dome. In an evaluation test of the resin composition that measures the shape change of the resin dome, H1 is defined as the height of the resin dome from the contact surface with the silicon wafer to the top of the resin dome 60 seconds after the distribution is completed, and H2 is defined as the height of the resin dome from the contact surface with the silicon wafer to the top of the resin dome 180 seconds after the distribution is completed. The following condition (1) is satisfied.

Description

Technical Field

[0001] This invention relates to resin compositions and syringes filled with resin compositions. Prior Technology

[0002] In recent years, the demand for small, high-performance electronic devices such as smartphones and tablets has been increasing. These small electronic devices typically use sealing materials for semiconductor chip packaging. As such sealing materials, those formed by curing resin compositions are known (Patent Documents 1-3).

[0003] Methods for molding sealing materials include melt injection molding, transfer molding, injection molding, and compression molding. In compression molding, for example, a syringe is used to distribute the resin composition onto a substrate, the mold is tightened, pressure is applied to the resin composition, and heat is applied if necessary, to perform compression molding. When distributing the resin composition using a syringe, good distribution and ejection workability are required from the perspective of improving workability. Furthermore, good resin flowability is required to prevent resin leakage from the mold during compression molding. However, these issues have not yet been adequately resolved simply by adjusting the thixotropy and viscosity of the resin composition.

[0004] Furthermore, syringes containing a pre-filled resin composition that can suppress air ingress that could cause intermittent ejection are known to exist (Patent Document 4). [Previous Technical Documents] [Patent Literature]

[0005] [Patent Document 1] Japanese Patent Application Publication No. 2004-137370 [Patent Document 2] Japanese Patent Application Publication No. 2012-188555 [Patent Document 3] Japanese Patent Application Publication No. 2016-74920 [Patent Document 4] Japanese Patent Application Publication No. 2020-127919 Summary of the Invention

[0006] [The problem the invention aims to solve]

[0007] The subject of this invention is to provide a resin composition with good distributability, dispensing properties and resin flowability, and a syringe filled with the resin composition. [Methods used to solve problems]

[0008] In order to achieve the purpose of this invention, the inventors, through active research, unexpectedly discovered that when a resin composition is distributed on the surface of a silicon wafer and a resin dome is formed, the shape of the resin dome changes over time to meet specific conditions, resulting in good distribution, extrusion workability, and resin flowability, thus completing this invention.

[0009] That is, the present invention includes the following. [1] A syringe filled with a resin composition, comprising a syringe and a resin composition filled within the syringe. Resin composition system A resin composition is distributed on the surface of a horizontally positioned silicon wafer to form a resin dome. An evaluation test of the resin composition, measuring the shape change of the resin dome, is conducted. Let H1 be the height of the resin dome from the contact surface with the silicon wafer to the top of the resin dome, 60 seconds after the distribution is completed. When the height of the resin dome from the contact surface with the silicon wafer to the apex of the resin dome is set to H2 180 seconds after the distribution is completed, The following condition (1) must be met. . [2] A syringe filled with a resin composition as described in [1] above, wherein the aforementioned evaluation test includes From the outlet located 5 cm above the surface of the silicon wafer, 40 g ± 1.5 g of resin composition at 23°C is distributed on the surface of the silicon wafer at a rate of 2 g / s under 23°C conditions, and the distribution stops to form a resin dome of the resin composition. [3] As described in [2] above, the syringe filled with the resin composition, wherein in the aforementioned evaluation test, When the distribution of the resin composition ceases and the outlet is no longer in contact with the resin dome, the point at which 40g ± 1.5g of resin composition has been distributed is taken as the aforementioned distribution completion point. When the dispensing nozzle comes into contact with the resin dome at the point when the distribution of the resin composition stops, the dispensing nozzle is pulled up after the distribution stops, and the dispensing nozzle is pulled away from the resin dome. The point when the dispensing nozzle leaves the resin dome is taken as the point when the aforementioned distribution is completed. [4] As described in any of [1] to [3] above, the diameter of the contact surface between the resin dome and the silicon wafer 60 seconds after the distribution is completed is defined as L1. When the diameter of the contact surface between the resin dome and the silicon wafer is set to L2 180 seconds after the distribution is completed, Therefore, the following condition (2) is satisfied. . [5] A syringe filled with a resin composition as described in any of [1] to [4] above, wherein the viscosity of the resin composition at 25°C is more than 100 Pa·s and less than 500 Pa·s. [6] A syringe filled with a resin composition as described in any of [1] to [5] above, wherein the resin composition comprises (A) a thermosetting resin. [7] A syringe filled with a resin composition as described in any of [1] to [6] above, wherein the resin composition includes (B) an inorganic filler. [8] A syringe filled with a resin composition as described in any of [1] to [7] above, wherein the resin composition contains (C) a silane coupling agent. [9] A resin composition is distributed on the surface of a horizontally arranged silicon wafer to form a resin dome. An evaluation test of the resin composition is conducted to measure the shape change of the resin dome. Let H1 be the height from the contact surface between the resin dome and the silicon wafer, 60 seconds after the distribution is completed, up to the apex of the resin dome. When H2 is defined as the height from the contact surface between the resin dome and the silicon wafer 180 seconds after the distribution completion point, to the apex of the resin dome, The following condition (1) must be met. .

[10] The resin composition as described in [9] above, wherein the aforementioned evaluation test includes, From the outlet located 5 cm above the surface of the silicon wafer, 40 g ± 1.5 g of resin composition at 23°C is distributed on the surface of the silicon wafer at a rate of 2 g / s under 23°C conditions, and the distribution stops to form a resin dome of the resin composition.

[11] The resin composition as described in

[10] above, wherein in the aforementioned evaluation test, When the distribution of the resin composition ceases and the outlet is no longer in contact with the resin dome, the point at which 40g ± 1.5g of resin composition has been distributed is taken as the aforementioned distribution completion point. When the outlet comes into contact with the resin dome at the point when the distribution of the resin composition stops, the outlet is pulled up after the distribution stops, and the outlet is pulled away from the resin dome. The point when the outlet leaves the resin dome is taken as the point when the aforementioned distribution is completed.

[12] The resin composition as described in any of [9] to

[11] above, wherein the diameter of the contact surface between the resin dome and the silicon wafer 60 seconds after the distribution is completed is set as L1. When the diameter of the contact surface between the resin dome and the silicon wafer is set to L2 180 seconds after the distribution is completed, Therefore, the following condition (2) is satisfied. .

[13] The resin composition of any one of [9] to

[12] above, wherein the viscosity of the resin composition at 25°C is more than 100 Pa·s and less than 500 Pa·s.

[14] The resin composition of any one of [9] to

[13] above, wherein the resin composition comprises (A) a thermosetting resin.

[15] A resin composition as described in any of [9] to

[14] above, wherein the resin composition comprises (B) an inorganic filler.

[16] A resin composition as described in any of [9] to

[15] above, wherein the resin composition comprises (C) a silane coupling agent.

[17] The resin composition of any of [9] to

[16] above is used to form an insulating layer for semiconductor wafer packaging.

[18] The resin composition of any one of [9] to

[16] above is used to form an insulating layer of a circuit board.

[19] The resin composition of any of [9] to

[16] above is used to seal the semiconductor wafer package.

[20] A cured product of a resin composition as described in any one of [9] to

[19] above.

[21] A circuit board comprising an insulating layer formed by a hardened resin composition as described in any one of [9] to

[19] above.

[22] A semiconductor wafer package comprising a circuit board as described above

[21] and a semiconductor wafer mounted on the circuit board.

[23] A semiconductor wafer package comprising a semiconductor wafer and a hardened resin composition as described in any one of [9] to

[19] above, sealing the semiconductor wafer.

[24] A semiconductor device having a semiconductor wafer package as described in

[22] or

[23] above.

[25] A method for evaluating a resin composition, comprising distributing a resin composition on the surface of a horizontally arranged silicon wafer to form a resin dome, and measuring the shape change of the resin dome, characterized by including Let H1 be the height from the contact surface between the resin dome and the silicon wafer, 60 seconds after the distribution is completed, up to the apex of the resin dome. When H2 is defined as the height from the contact surface between the resin dome and the silicon wafer 180 seconds after the distribution completion point, to the apex of the resin dome, Determine whether the following condition (1) is met. . [Invention Effects]

[0010] According to the resin composition of the present invention, a resin composition with good distributability, dispensing performance and resin flowability, and a syringe filled with the resin composition can be provided. Simple Explanation of the Diagram

[0011] [Figure 1] is a cross-sectional view schematically showing an example of a syringe filled with a resin composition according to one embodiment of the present invention. [Figure 2] is a schematic cross-sectional view showing an example of a nozzle installed in a syringe filled with a resin composition according to one embodiment of the present invention. [Figure 3] is a schematic cross-sectional view from the horizontal direction of the resin dome formed on the silicon wafer at the point of completion of the distribution during an evaluation test of an embodiment, together with a part of the syringe filled with the resin composition. [Figure 4] is a schematic cross-sectional view of the resin dome formed on the silicon wafer at the point of completion of the distribution in an evaluation test of an embodiment, viewed from the vertical direction. Implementation

[0012] The present invention will now be described in detail based on preferred embodiments. However, the present invention is not limited to the embodiments and examples described below, and any modifications may be made without departing from the scope of the claims and their equivalents.

[0013] <Instrument filled with resin> The syringe filled with a resin composition of the present invention comprises a syringe and a resin composition filled in the syringe.

[0014] An example of the configuration and use of the syringe filled with the resin composition of the present invention and the nozzle installed thereon will be described. FIG1 is a schematic cross-sectional view showing an example of the syringe filled with the resin composition of one embodiment of the present invention. FIG2 is a schematic cross-sectional view showing an example of the nozzle installed in the syringe filled with the resin composition of one embodiment of the present invention.

[0015] As shown in Figure 1, the syringe 10 filled with resin composition includes a syringe 11, a resin composition 12 filled within the syringe 11, and a plunger 13 for extruding the resin composition 12 within the syringe 11. Furthermore, the syringe 10 filled with resin composition has a female thread 14 formed by threaded teeth on the inner surface of one end of the syringe 11 with a reduced diameter for mounting a nozzle 20. At the tip of this end is an outlet 15 for discharging the resin composition. At the other end, opposite to the outlet 15, is an opening 16 for inserting a plunger rod. The outlet 15 has a front cap 17 that covers the outlet 15 and is removed during use. The opening 16 has a rear cap 18 that covers the opening 16 and is removed during use.

[0016] In one embodiment, the syringe 11 can be a distribution syringe that can be used as a sealing material that can be filled with the resin composition of the present invention; a "12oz syringe" is particularly preferred. Examples of commercially available "12oz syringes" include, for instance, the "5194C" manufactured by SAN-EI TECH. The "12oz syringe" may have an inner diameter of 14.22 mm and an outer diameter of 19.30 mm for the nozzle 15, an inner diameter of 40.26 mm for the opening 16, and a length of 311.40 mm from the nozzle 15 to the opening 16.

[0017] The syringe 10 filled with resin composition is sometimes used with a nozzle 20 installed. When the nozzle 20 is installed in the syringe 10 filled with resin composition, the front cap 17 is removed. As shown in FIG2, the nozzle 20 is composed of a tube 21 and a syringe connector 22, and a portion of the tube 21 is inserted into the syringe connector 22 and fixed therein. The tip of the tube 21 has a nozzle ejection portion 23 for ejecting the resin composition, and at the other end of the syringe connector 22, when the nozzle 20 is fixed to the syringe 10 filled with resin composition, there is a nozzle opening 24 for feeding the resin composition 12 into the syringe 11, and the whole is tubular. On the outer surface of the other end of the syringe connector 22, there is a male thread portion 25 formed by threads, which engages with a female thread portion 14 for installing and fixing the nozzle 20 to the syringe 10 filled with resin composition. The tube 21 is formed of a soft material, and has a structure that can be squeezed by external pressure to stop the distribution of the resin composition.

[0018] <Resin Composition and its Evaluation Tests (Evaluation Methods)> The resin composition used in this invention satisfies the conditions of formula (1) described below (preferably the conditions of formula (2)) in the evaluation test results of the resin composition described below.

[0019] The following describes the evaluation tests (evaluation methods) for resin components.

[0020] In the evaluation test for resin composition evaluation, the resin composition is distributed on the surface of a horizontally set silicon wafer to form a resin dome of the resin composition. The shape change of the resin dome is measured to determine whether it meets the conditions of Equation (1) as described below (preferably Equation (2)).

[0021] In the evaluation test, a syringe can also be used for distribution through the syringe nozzle. The syringe used in the evaluation test can be, for example, a syringe 10 filled with resin composition as shown in Figure 1. During distribution, the front cap 17 and rear cap 18 of the syringe are removed. When measuring the distribution with respect to the resin dome shape under the specific conditions described below, the nozzle 20 may or may not be installed. In the evaluation test, a conventional distributor is used for distribution. An example of a commercially available distributor used in the evaluation test is... "Liquid Manual Distributor" manufactured by APICYAMADA.

[0022] For the silicon wafers used in the evaluation test, silicon wafers with an arithmetic mean roughness (Ra) of 10 Å or less can be used, and there are no particular restrictions on the size as long as the evaluation test can be performed.

[0023] The distribution of resin dome formation in an evaluation test of one embodiment will be illustrated using schematic diagrams. Figure 3 is a schematic cross-sectional view, viewed horizontally, showing a portion of the syringe filled with the resin composition, at the point when the distribution is complete in an evaluation test of one embodiment. Figure 4 is a schematic cross-sectional view, viewed vertically, showing the resin dome formation on the silicon wafer at the point when the distribution is complete in an evaluation test of one embodiment.

[0024] In this embodiment, an syringe without a nozzle is used in the evaluation test. In this embodiment, the case where the nozzle 20 is not installed, as in Test Example 3 below, will be described. As shown in Figure 3, firstly, a syringe 10 with the front cover 17 and rear cover 18 removed and filled with resin composition is installed such that the height Hs from the surface of the horizontally set silicon wafer 40 to the outlet 15 is 5 cm.

[0025] Next, in this embodiment, the syringe 10, which is self-filled with resin composition, distributes 40g ± 1.5g of resin composition (at the same temperature as the outside air) onto the silicon wafer surface at a rate of 2g / s under 23°C conditions. Distribution is stopped at the point where 40g ± 1.5g of resin composition has been distributed, forming a resin dome 20. "Stopping distribution" means cutting off the supply of resin composition to the silicon wafer surface by stopping the plunger, blocking the outlet (nozzle outlet), or blocking the nozzle tube when the nozzle is in use. In this embodiment, since distribution is stopped at the point where 40g ± 1.5g of resin composition has been distributed, the amount of resin composition in the resin dome 20 is 40g ± 1.5g.

[0026] Furthermore, in this embodiment, when the outlet comes into contact with the resin dome at the point when the distribution of the resin composition stops, the outlet is pulled up after the distribution stops, and an operation is performed to pull the outlet away from the resin dome.

[0027] Furthermore, in this embodiment, when the outlet is not in contact with the resin dome at the point when the distribution of the resin composition stops, the point when the resin composition has been distributed to 40g±1.5g is taken as the distribution completion point. When the outlet is in contact with the resin dome at the point when the distribution of the resin composition stops, the outlet is pulled up after the distribution stops, and the outlet is pulled away from the resin dome. The point when the outlet leaves the resin dome is taken as the distribution completion point.

[0028] The resin dome 30 of the resin composition, as shown in FIG. 3, is a dome-shaped mass of the liquid resin composition. Since the resin composition usually spreads circularly with the dropping point of the resin composition as the center, as shown in FIG. 4, the contact surface with the silicon wafer 40 can be circular.

[0029] The resin dome 30 of the resin composition usually spreads circularly with the dropping point of the resin composition as the center over time after distribution. Therefore, the height H0 from the contact surface of the resin dome 30 with the silicon wafer 40 to the apex of the resin dome becomes lower over time. Thus, as a specific first condition indicating the change over time of the shape of the resin dome 30, for the resin composition of the present invention, when the height (distance in the direction perpendicular to the surface of the silicon wafer 40) from the contact surface of the resin dome 30 with the silicon wafer 40 to the apex of the resin dome at 60 seconds after the completion of distribution is set as H1, and the height (distance in the direction perpendicular to the surface of the silicon wafer 40) from the contact surface of the resin dome 20 with the silicon wafer 30 to the apex of the resin dome at 180 seconds after the completion of distribution is set as H2, the condition of the following formula (1) is satisfied. 。

[0030] Under the condition of the above formula (1), H2 / H1 satisfies 0.15 < H2 / H1, preferably 0.20 < H2 / H1, more preferably 0.25 < H2 / H1, still more preferably 0.30 < H2 / H1, and particularly preferably 0.33 < H2 / H1. On the other hand, H2 / H1 satisfies H2 / H1 < 0.90, preferably H2 / H1 < 0.85, and particularly preferably H2 / H1 < 0.82.

[0031] The resin composition of the present invention, by satisfying the condition of the above formula (1), can have the characteristic of good distribution in one embodiment. Since the distribution is good, it can be smoothly discharged from the discharge port 15 (nozzle discharge part 23) of the syringe 10 for self-filling the resin composition. Since it is difficult to generate a backflow phenomenon, the operability can be good.

[0032] Moreover, the resin composition of the present invention, by satisfying the conditions of the above formula (1), may have the characteristic of good discharge workability in one embodiment. Since the discharge workability is good, the liquid throwing property is good, it is difficult to cause liquid separation or resin collapse, and the resin composition can be distributed with an accurate resin supply amount. The so-called liquid throwing property refers to the property of quickly stopping the discharge of the resin composition from the discharge part 23 of the nozzle when the distribution stops. Moreover, the so-called liquid separation refers to the property that the resin composition flowing out from the discharge part 23 of the nozzle does not adhere to the discharge port 15 and is easily separated.

[0033] Furthermore, the resin composition of the present invention, by satisfying the conditions of the above formula (1), may have the characteristic of good resin fluidity in one embodiment. Since the resin fluidity is good, it is difficult to generate unfilled parts in the mold, and since it is difficult for the resin to leak from the mold during compression molding, the compression molding property can be excellent.

[0034] Moreover, the diameter L0 of the contact surface of the resin dome 30 with the silicon wafer 40 increases with time after the distribution. Thus, as a specific second condition indicating the change in the shape of the resin dome 30 with time, for the resin composition of the present invention, when the diameter of the contact surface of the resin dome 30 with the silicon wafer 40 at 60 seconds after the completion of the distribution is set as L1 and the diameter of the contact surface of the resin dome 30 with the silicon wafer 40 at 180 seconds after the completion of the distribution is set as L2, it is preferably further to satisfy the conditions of the following formula (2). 。

[0035] Under the conditions of the above formula (2), L1 / L2 satisfies 0.40 < L1 / L2, preferably 0.45 < L1 / L2, particularly preferably 0.48 < L1 / L2. On the other hand, L1 / L2 satisfies L1 / L2 < 0.96, preferably L1 / L2 < 0.94, more preferably L1 / L2 < 0.92, particularly preferably L1 / L2 < 0.90.

[0036] The resin composition of the present invention, by satisfying the conditions of the above formula (2), may further improve the distribution property, discharge workability and resin fluidity of the resin composition in one embodiment.

[0037] Furthermore, 180 seconds after the completion of the distribution, the conditions are the same as those during the distribution at 23°C.

[0038] Based on the viewpoint of improving resin fluidity and preventing resin leakage from the mold during compression molding, the viscosity of the resin composition of the present invention at 25°C is generally 1 Pa·s or more, preferably 2.5 Pa·s or more, 10 Pa·s or more, more preferably 30 Pa·s or more, 50 Pa·s or more, even more preferably 80 Pa·s or more, 90 Pa·s or more, even more preferably 100 Pa·s or more, 110 Pa·s or more, and particularly preferably 120 Pa·s or more, 130 Pa·s or more. Furthermore, the upper limit of the viscosity of the resin composition at 25°C, based on the viewpoint of improving distribution and preventing backflow, is typically below 2000 Pa·s, preferably below 1000 Pa·s or 900 Pa·s, preferably below 800 Pa·s or 700 Pa·s, preferably below 650 Pa·s or 600 Pa·s, preferably below 500 Pa·s or 450 Pa·s, and particularly preferably below 400 Pa·s or 380 Pa·s. The aforementioned viscosity can be measured using an E-type viscometer.

[0039] The resin composition of the present invention may contain components selected from (A) thermosetting resins, (B) inorganic fillers, (C) free radical polymerizable compounds, (D) free radical polymerization initiators, (E) thermoplastic resins, (F) curing accelerators, (G) compounds containing polyether skeletons, (H) other additives, and (I) organic solvents. Those skilled in the art can adjust the resin composition to satisfy the conditions of formulas (1) and (2) above by selecting these components and changing their contents. Hereinafter, each component contained in the resin composition will be described in detail.

[0040] <(A) Thermosetting Resin> The resin composition of this invention may contain (A) a thermosetting resin. The thermosetting resin may be a thermosetting resin suitable for use as a sealing material in electronic devices. Examples of (A) thermosetting resins include epoxy resins, epoxy acrylate resins, urethane acrylate resins, urethane resins, cyanate ester resins, benzoxazine resins, unsaturated polyester resins, phenolic resins, melamine resins, and silicone resins.

[0041] <(A-1) Epoxy Resin> The resin composition of the present invention, as (A) a thermosetting resin, may contain (A-1) an epoxy resin. (A-1) An epoxy resin refers to a resin having epoxy groups.

[0042] Examples of (A-1) epoxy resins include, for example, xylenol-type epoxy resin, bisphenol A-type epoxy resin, bisphenol F-type epoxy resin, bisphenol S-type epoxy resin, bisphenol AF-type epoxy resin, dicyclopentadiene-type epoxy resin, triphenol-type epoxy resin, naphthol phenolic varnish-type epoxy resin, phenolic phenolic varnish-type epoxy resin, tributyl-catechol-type epoxy resin, naphthalene-type epoxy resin, naphthol-type epoxy resin, anthracene-type epoxy resin, glycidylamine-type epoxy resin, glycidyl ester-type epoxy resin, cresol phenolic varnish-type epoxy resin, biphenyl-type epoxy resin, chain aliphatic epoxy resin, epoxy resin having a butadiene structure, alicyclic epoxy resin, heterocyclic epoxy resin, epoxy resin containing spirocyclic rings, cyclohexane-type epoxy resin, cyclohexanediethanol-type epoxy resin, naphthyl ether-type epoxy resin, trihydroxymethyl-type epoxy resin, and tetraphenylethane-type epoxy resin. Epoxy resin can be used alone or in combination with two or more types.

[0043] In the resin composition of the present invention, the (A-1) epoxy resin preferably comprises an epoxy resin having two or more epoxy groups per molecule. From the viewpoint of significantly achieving the desired effects of the present invention, the proportion of epoxy resin having two or more epoxy groups per molecule relative to 100% by mass of the non-volatile component of the (A-1) epoxy resin is preferably 50% by mass or more, more preferably 60% by mass or more, and particularly preferably 70% by mass or more.

[0044] (A-1) Epoxy resins include epoxy resins that are liquid at 25°C (hereinafter sometimes referred to as "liquid epoxy resins") and epoxy resins that are solid at 25°C (hereinafter sometimes referred to as "solid epoxy resins"). In the resin composition of the present invention, the (A-1) epoxy resin may contain only solid epoxy resin, or only liquid epoxy resin, or a combination of liquid and solid epoxy resins, but it is more preferably to contain liquid epoxy resin. It is particularly preferred that the (A-1) epoxy resin contains only liquid epoxy resin.

[0045] The preferred liquid epoxy resin is a liquid epoxy resin having two or more epoxy groups in one molecule.

[0046] As liquid epoxy resins, glycyrrhizic acid type epoxy resins, bisphenol A type epoxy resins, bisphenol F type epoxy resins, bisphenol AF type epoxy resins, naphthalene type epoxy resins, glycidyl ester type epoxy resins, glycidyl amine type epoxy resins, phenolic varnish type epoxy resins, alicyclic epoxy resins with an ester skeleton, cyclohexanediol type epoxy resins, cyclic aliphatic glycidyl ethers, and epoxy resins with a butadiene structure are preferred. Glycyrrhizic acid type epoxy resins, cyclic aliphatic glycidyl ethers, bisphenol A type epoxy resins, and bisphenol F type epoxy resins are even more preferred.

[0047] Specific examples of liquid epoxy resins include NAGASE CHEMTEX's "EX-992L"; Mitsubishi Chemical's "YX7400"; DIC's "HP4032", "HP4032D", and "HP4032SS" (naphthalene-type epoxy resin); and Mitsubishi Chemical's "828US", "828EL", "jER828EL", "825", and "EPICOTE". 828EL (Bisphenol A type epoxy resin); Mitsubishi Chemical's "jER807" and "1750" (Bisphenol F type epoxy resin); Mitsubishi Chemical's "jER152" (Phenolic varnish type epoxy resin); Mitsubishi Chemical's "630", "630LSD", and "604" (Glycidylamine type epoxy resin); ADEKA's "ED-523T" (Glycyrrhizic acid type epoxy resin); ADEKA's "EP-3950L" and "EP-3980S" (Glycidylamine type epoxy resin); ADEKA's "EP-4088S" (Dicyclopentadiene type epoxy resin); Nippon Steel Chemical & Materials Co., Ltd.'s "ZX1059" (a mixture of bisphenol A type epoxy resin and bisphenol F type epoxy resin); NAGASE CHEMTEX's "EX-721" (glycidyl ester type epoxy resin); NAGASE CHEMTEX's "EX-991L" (epoxy resin containing alkoxy groups); DAICEL's "CELOXIDE 2021P" (alicyclic epoxy resin with an ester skeleton); DAICEL's "PB-3600"; Nippon Soda's "JP-100" and "JP-200" (epoxy resins with butadiene structures); Nippon Steel Chemicals & Materials' "ZX1658" and "ZX1658GS" (liquid 1,4-glycidylcyclohexane type epoxy resin); Osaka Gas Chemicals' "EG-280" (epoxy resin with a cyclohexane structure); NAGASE CHEMTEX's "EX-201" (cyclic aliphatic glycidyl ether), etc.

[0048] The solid epoxy resin is preferably a solid epoxy resin having three or more epoxy groups per molecule, and more preferably an aromatic solid epoxy resin having three or more epoxy groups per molecule.

[0049] Preferred solid epoxy resins include bixylenol-type epoxy resins, naphthalene-type epoxy resins, naphthalene-type tetrafunctional epoxy resins, naphthol phenolic varnish-type epoxy resins, cresol phenolic varnish-type epoxy resins, dicyclopentadiene-type epoxy resins, triphenol-type epoxy resins, naphthol-type epoxy resins, biphenyl-type epoxy resins, naphthyl ether-type epoxy resins, anthracene-type epoxy resins, bisphenol A-type epoxy resins, bisphenol AF-type epoxy resins, phenol aralkyl-type epoxy resins, tetraphenylethane-type epoxy resins, phenol phthalamide-type epoxy resins, and phenolphthalein-type epoxy resins.

[0050] Specific examples of solid epoxy resins include DIC's "HP4032H" (naphthalene-type epoxy resin); DIC's "HP-4700" and "HP-4710" (naphthalene-type tetrafunctional epoxy resins); DIC's "N-690" (cresol-phenolic varnish type epoxy resin); DIC's "N-695" (cresol-phenolic varnish type epoxy resin); and DIC's "HP-7200," "HP-7200HH," "HP-7200H," and "HP-7200L" (dicyclopentadiene type epoxy resins). Company C manufactures "EXA-7311", "EXA-7311-G3", "EXA-7311-G4", "EXA-7311-G4S", and "HP6000" (naphthalene ether type epoxy resin); Nippon Kayaku Co., Ltd. manufactures "EPPN-502H" (triphenol type epoxy resin); Nippon Kayaku Co., Ltd. manufactures "NC7000L" (naphthalene phenolic varnish epoxy resin); Nippon Kayaku Co., Ltd. manufactures "NC3000H", "NC3000", "NC3000L", "NC3000FH", and "NC3100" (biphenyl type epoxy resin). Nippon Steel Chemicals & Materials Co., Ltd.'s "ESN475V" (naphthalene-type epoxy resin); Nippon Steel Chemicals & Materials Co., Ltd.'s "ESN485" (naphthol-type epoxy resin); Nippon Steel Chemicals & Materials Co., Ltd.'s "ESN375" (dihydroxynaphthalene-type epoxy resin); Mitsubishi Chemical Corporation's "YX4000H", "YX4000", "YX4000HK", and "YL7890" (bi-xylenol-type epoxy resin); Mitsubishi Chemical Corporation's "YL6121" (biphenyl-type epoxy resin); Mitsubishi Chemical Corporation's "YX8800" (anthracite-type epoxy resin); The following epoxy resins are available from Mitsubishi Chemical Corporation: "YX7700" (phenolic alkyl type epoxy resin); "PG-100" and "CG-500" from Osaka Gas Chemical Co., Ltd.; "YL7760" (bisphenol AF type epoxy resin) from Mitsubishi Chemical Corporation; "YL7800" (bisphenol A type epoxy resin) from Mitsubishi Chemical Corporation; "jER1010" (bisphenol A type epoxy resin) from Mitsubishi Chemical Corporation; "jER1031S" (tetraphenylethane type epoxy resin) from Mitsubishi Chemical Corporation; and "WHR991S" (phenolic phthalamide type epoxy resin) from Nippon Kayaku Co., Ltd. These resins can be used alone or in combination of two or more.

[0051] (A-1) The epoxy equivalent of the epoxy resin is preferably 50 g / eq. to 5000 g / eq., more preferably 50 g / eq. to 3000 g / eq., even more preferably 80 g / eq. to 2000 g / eq., and still more preferably 110 g / eq. to 1000 g / eq. The epoxy equivalent is the resin mass per equivalent of epoxy groups. This epoxy group equivalent can be determined according to JIS K7236.

[0052] (A-1) The weight-average molecular weight (Mw) of the epoxy resin is preferably 100-5000, more preferably 250-3000, and even more preferably 400-1500, based on the viewpoint of significantly achieving the intended effects of the present invention. The weight-average molecular weight of the resin is determined by gel permeation chromatography (GPC) using a polystyrene equivalent.

[0053] The content of epoxy resin (A-1) in the resin composition is not particularly limited, but when all non-volatile components in the resin composition are set as 100% by mass, it is, for example, 0% or more by mass, 0.01% or more by mass, preferably 0.1% or more by mass, more preferably 1% or more by mass, particularly preferably 3% or more by mass, preferably 30% or less by mass, more preferably 20% or less by mass, and particularly preferably 15% or less by mass. When the non-volatile components other than inorganic fillers (B) in the resin composition are set as 100% by mass, it is, for example, 0% or more by mass, 1% or more by mass, preferably 10% or more by mass, more preferably 20% or more by mass, particularly preferably 30% or more by mass, preferably 90% or less by mass, more preferably 85% or less by mass, and particularly preferably 80% or less by mass.

[0054] <(A-2) Epoxy Curing Agent> When the resin composition of the present invention contains (A-1) epoxy resin as (A) thermosetting resin, it may further contain (A-2) epoxy curing agent as an optional component. The (A-2) epoxy curing agent has the function of reacting with (A-1) epoxy resin to cure the resin composition as an epoxy resin curing agent.

[0055] The epoxy curing agent in (A-2) is not particularly limited, but examples include reactive ester-based curing agents, phenolic curing agents, carbodiimide-based curing agents, acid anhydride-based curing agents, amine-based curing agents, benzoxazine-based curing agents, cyanate ester-based curing agents, and thiol-based curing agents. One type of epoxy curing agent in (A-2) may be used alone, or two or more may be used in combination. Preferably, the epoxy curing agent in (A-2) includes epoxy curing agents selected from reactive ester-based curing agents and phenolic curing agents.

[0056] As an active ester-based curing agent, it is generally preferred to use compounds such as phenolic esters, thiophenolic esters, N-hydroxyamine esters, and heterocyclic hydroxyl compounds, which have two or more highly reactive ester groups in one molecule.

[0057] Reactive ester-based curing agents are preferably obtained through the condensation reaction of carboxylic acid compounds and / or thiocarboxylic acid compounds with hydroxyl compounds and / or thiols. Especially from the viewpoint of improving heat resistance, reactive ester-based curing agents obtained from carboxylic acid compounds and hydroxyl compounds are preferred, and even more preferred are reactive ester-based curing agents obtained from carboxylic acid compounds and phenolic compounds and / or naphthol compounds.

[0058] Examples of active ester-based curing agents include benzoic acid, acetic acid, succinic acid, maleic acid, itaconic acid, phthalic acid, isophthalic acid, terephthalic acid, and pyromellitic acid. Examples of phenolic or naphthol compounds include hydroquinone, resorcinol, bisphenol A, bisphenol F, bisphenol S, phenolphthalein, methylated bisphenol A, methylated bisphenol F, methylated bisphenol S, phenol, o-cresol, m-cresol, p-cresol, catechol, α-naphthol, β-naphthol, 1,5-dihydroxynaphthol, 1,6-dihydroxynaphthol, 2,6-dihydroxynaphthol, dihydroxybenzophenone, trihydroxybenzophenone, tetrahydroxybenzophenone, phloroglucin, pyrogallol, dicyclopentadiene-type bisphenol compounds, and phenolic varnishes. Here, "dicyclopentadiene-type diphenol compounds" refers to diphenol compounds obtained by condensing 2 phenol molecules into 1 molecule of dicyclopentadiene.

[0059] Specifically, the preferred active ester-based curing agent is a dicyclopentadiene-type active ester-based curing agent, a naphthalene-type active ester-based curing agent containing a naphthalene structure, an active ester-based curing agent containing an acetylene compound of phenolic varnish, or an active ester-based curing agent containing a benzoylene compound of phenolic varnish. More preferably, it is selected from at least one of dicyclopentadiene-type and naphthalene-type active ester-based curing agents. As a dicyclopentadiene-type active ester-based curing agent, it is more preferably an active ester-based curing agent containing a dicyclopentadiene-type diphenol structure.

[0060] Commercially available reactive ester curing agents include, for example, those containing a dicyclopentadiene-type bisphenol structure such as "EXB9451", "EXB9460", "EXB9460S", "EXB-8000L", "EXB-8000L-65M", "EXB-8000L-65TM", "HPC-8000L-65TM", "HPC-8000", "HPC-8000-65T", "HPC-8000H", and "HPC-8000H-65TM" (manufactured by DIC Corporation); and those containing a naphthalene structure such as "EXB-8151-62T", "EXB-8100L-65T", and "EXB-8150". Examples of active ester curing agents include "-60T", "EXB-8150-62T", "EXB-9416-70BK", "HPC-8150-60T", and "HPC-8150-62T" (manufactured by DIC Corporation); examples of phosphorus-containing active ester curing agents include "EXB9401" (manufactured by DIC Corporation); examples of active ester curing agents for acetylated phenolic varnishes include "DC808" (manufactured by Mitsubishi Chemical Corporation); examples of active ester curing agents for benzoyl compounds in phenolic varnishes include "YLH1026", "YLH1030", and "YLH1048" (manufactured by Mitsubishi Chemical Corporation); and examples of active ester curing agents containing styrene and naphthalene structures include "PC1300-02-65MA" (manufactured by AIR WATER Corporation).

[0061] Examples of phenolic curing agents include those having one or more, preferably two or more, hydroxyl groups bonded to aromatic rings such as benzene or naphthalene rings in one molecule. Among these, compounds having hydroxyl groups bonded to benzene rings are preferred.

[0062] Specific examples of phenolic curing agents include: MEH-7700, MEH-7810, MEH-7851, and MEH-8000H manufactured by Meiwa Chemical Co., Ltd.; NHN, CBN, and GPH manufactured by Nippon Kayaku Co., Ltd.; TD-2090, TD-2090-60M, LA-7052, LA-7054, LA-1356, LA-3018, LA-3018-50P, EXB-9500, HPC-9500, KA-1160, KA-1163, and KA-1165 manufactured by DIC Co., Ltd.; GDP-6115L, GDP-6115H, and ELPC75 manufactured by Kunei Chemical Co., Ltd.; and SIGMA. "2,2-Dearly allyl bisphenol A" manufactured by ALDRICH, etc.

[0063] Examples of carbodiimide-based curing agents include those having one or more, preferably two or more, carbodiimide structures within one molecule. Examples include aliphatic bis(tert-butylcarbodiimide) and cyclohexanebis(methylene-tert-butylcarbodiimide); aromatic bis(xylenecarbodiimide); and aliphatic poly(hexamethylenecarbodiimide), trimethylhexamethylenecarbodiimide, polycyclohexylcarbodiimide, poly(methylenebiscyclohexylcarbodiimide), and poly(isophoronecarbodiimide). Carbodiimides; poly(phenylcarbodiimide), poly(naphthylcarbodiimide), poly(toluenecarbodiimide), poly(methyldiisopropylphenylcarbodiimide), poly(triethylphenylcarbodiimide), poly(diethylphenylcarbodiimide), poly(triisopropylphenylcarbodiimide), poly(diisopropylphenylcarbodiimide), poly(xylylcarbodiimide), poly(tetramethylxylylcarbodiimide), poly(methylenediphenylcarbodiimide), poly[methylenebis(methylphenyl)carbodiimide] and other aromatic polycarbodiimides and other polycarbodiimides.

[0064] Commercially available products as carbodiimide curing agents include, for example, "CARBODILITE V-02B", "CARBODILITE V-03", "CARBODILITE V-04K", "CARBODILITE V-07" and "CARBODILITE V-09" manufactured by Nisshinbo Chemical Co., Ltd.; and "STABAXOL P", "STABAXOL P400" and "HYCAZIL 510" manufactured by LANXESS Chemical Co., Ltd.

[0065] Anhydride-based curing agents include, for example, curing agents having one or more anhydride groups per molecule, preferably curing agents having two or more anhydride groups per molecule. Specific examples of anhydride-based curing agents include phthalic anhydride, tetrahydrophthalic anhydride, hexahydrophthalic anhydride, methyltetrahydrophthalic anhydride, methylhexahydrophthalic anhydride, methyl terephthalic anhydride, hydrogenated methyl terephthalic anhydride, trialkyltetrahydrophthalic anhydride, dodecenylsuccinic anhydride, 5-(2,5-dioxotetrahydro-3-furanyl)-3-methyl-3-cyclohexene-1,2-dicarboxylic anhydride, phenyltrisuccinic anhydride, pyromellitic anhydride, and diphenyl Polymer anhydrides such as methyl ketone tetracarboxylic anhydride, biphenyl tetracarboxylic anhydride, naphthalene tetracarboxylic anhydride, oxydiphthalic anhydride, 3,3',4,4'-diphenyltristyrene tetracarboxylic anhydride, 1,3,3a,4,5,9b-hexahydro-5-(tetrahydro-2,5-dioxo-3-furanyl)-naphtho[1,2-C]-furan-1,3-dione, ethylene glycol bis(phenyltriacyl anhydride), and styrene-maleic acid resin copolymerized with styrene and maleic acid. Commercially available anhydride-based curing agents include, for example, "HNA-100", "MH-700", "MTA-15", "DDSA", and "OSA" manufactured by New Japan Rika Co., Ltd.; "YH-306" and "YH-307" manufactured by Mitsubishi Chemical Co., Ltd.; and "HN-2200" and "HN-5500" manufactured by Hitachi Chemical Co., Ltd.

[0066] Examples of amine-based curing agents include those having one or more, preferably two or more, amine groups per molecule. Examples include aliphatic amines, polyether amines, alicyclic amines, and aromatic amines. From the viewpoint of achieving the desired effect of this invention, aromatic amines are preferred. The amine-based curing agent is preferably a primary or secondary amine, more preferably a primary amine. Specific examples of amine-based curing agents include 4,4'-methylenebis(2,6-dimethylaniline), 4,4'-diaminodiphenylmethane, 4,4'-diaminodiphenyl sulfone, 3,3'-diaminodiphenyl sulfone, m-phenylenediamine, m-xylenediamine, diethyltoluenediamine, 4,4'-diaminodiphenyl ether, 3,3'-dimethyl-4,4'-diaminobiphenyl, 2,2'-dimethyl-4,4'-diaminobiphenyl, 3,3'-dihydroxybenzidine, and 2,2-bis(3-amino-4-hydroxy) 2,2-bis(4-aminophenyl)propane, 3,3-dimethyl-5,5-diethyl-4,4-diphenylmethanediamine, 2,2-bis(4-aminophenyl)propane, 2,2-bis(4-(4-aminophenoxy)phenyl)propane, 1,3-bis(3-aminophenoxy)benzene, 1,3-bis(4-aminophenoxy)benzene, 1,4-bis(4-aminophenoxy)benzene, 4,4'-bis(4-aminophenoxy)biphenyl, bis(4-(4-aminophenoxy)phenyl) benzoxide, bis(4-(3-aminophenoxy)phenyl) benzoxide, etc. Amine-based hardeners can also be commercially available products, such as SEIKA's "SEIKACURE-S", Nippon Kayaku Co., Ltd.'s "KAYABOND C-200S", "KAYABOND C-100", "KAYAHARD AA", "KAYAHARD AB", "KAYAHARD AS", and Mitsubishi Chemical's "EPICURE W".

[0067] Specific examples of benzoxazine-based hardeners include "JBZ-OP100D" and "ODA-BOZ" manufactured by JFE Chemical Co., Ltd.; "HFB2006M" manufactured by Showa Polymer Co., Ltd.; and "Pd" and "Fa" manufactured by Shikoku Chemical Co., Ltd.

[0068] Examples of cyanate ester-based curing agents include, for instance, bisphenol A dicyanate, polyphenol cyanates (oligomeric (3-methylene-1,5-phenyl cyanate)), 4,4'-methylenebis(2,6-dimethylphenyl cyanate), 4,4'-ethylidene diphenyl dicyanate, hexafluorobisphenol A dicyanate, 2,2-bis(4-cyanate-phenyl)propane, 1,1-bis(4-cyanate-phenylmethane), bis(4-cyanate-3,5-dimethylphenyl)methane, 1,3-bis(4-cyanate-phenyl-1-(methylethylidene))benzene, bis(4-cyanate-phenyl) sulfide, and bis(4-cyanate-phenyl) ether, etc., difunctional cyanate ester resins, polyfunctional cyanate ester resins derived from phenolic varnishes and cresol varnishes, etc., and prepolymers formed by partially triazinizing such cyanate ester resins, etc. Specific examples of cyanate ester-based curing agents include "PT30" and "PT60" (both phenolic varnish-type multifunctional cyanate ester resins), "BA230", and "BA230S75" (prepolymers of trimers in which some or all of bisphenol A dicyanate has been triazineized), manufactured by LONZA Corporation of Japan.

[0069] Examples of thiol-based curing agents include trimethylolpropane tris(3-mercaptopropionate), pentaerythritol tetra(3-mercaptobutyrate), and tris(3-mercaptopropyl)isocyanurate.

[0070] (A-2) The reactive base equivalent of the epoxy curing agent is preferably 50 g / eq. to 3000 g / eq., more preferably 100 g / eq. to 1000 g / eq., even more preferably 100 g / eq. to 500 g / eq., and particularly preferably 100 g / eq. to 300 g / eq. The reactive base equivalent refers to the mass of curing agent per 1 equivalent of reactive base.

[0071] The content of epoxy curing agent (A-2) in the resin composition is not particularly limited, but when all non-volatile components in the resin composition are set to 100% by mass, for example, it is 0% or more by mass, 0.01% or more by mass, preferably 0.1% or more by mass, more preferably 1% or more by mass, particularly preferably 2% or more by mass, preferably 20% or less by mass, more preferably 10% or less by mass, and particularly preferably 7% or less by mass. When the non-volatile components other than inorganic filler (B) in the resin composition are set to 100% by mass, for example, it is 0% or more by mass, 0.1% or more by mass, preferably 1% or more by mass, more preferably 5% or more by mass, particularly preferably 10% or more by mass, preferably 80% or less by mass, more preferably 70% or less by mass, and particularly preferably 60% or less by mass.

[0072] <(B) Inorganic filler> The resin composition of the present invention may contain (B) inorganic filler as any component.

[0073] The material used as (B) inorganic filler is an inorganic compound. Examples of inorganic filler materials include silicon oxide, aluminum oxide, glass, cordierite, silicon oxide, barium sulfate, barium carbonate, talc, clay, mica powder, zinc oxide, hydrotalcite, boehmite, aluminum hydroxide, magnesium hydroxide, calcium carbonate, magnesium carbonate, magnesium oxide, boron nitride, aluminum nitride, manganese nitride, aluminum borate, strontium carbonate, strontium titanate, calcium titanate, magnesium titanate, bismuth titanate, titanium oxide, zirconium oxide, barium titanate, barium zirconate titanate, barium zirconate, calcium zirconate, zirconium phosphate, and zirconium tungstate phosphate. Among these, silicon oxide is particularly preferred. Examples of silicon oxide include amorphous silicon oxide, molten silicon oxide, crystalline silicon oxide, synthetic silicon oxide, and hollow silicon oxide. Spherical silicon oxide is preferred as the silicon oxide. (B) Inorganic fillers can be used alone or in combination of two or more.

[0074] (B) The 50% cumulative diameter D50 of the inorganic filler is preferably 0.2 μm or more, more preferably 0.3 μm or more, particularly preferably 0.4 μm or more, preferably 15 μm or less, more preferably 12 μm or less, and even more preferably 10 μm or less. (B) If the 50% cumulative diameter D50 of the inorganic filler is too small, the distribution will be reduced, and backflow may easily occur.

[0075] (B) The 90% cumulative diameter D90 of the inorganic filler is preferably 2 μm or more, more preferably 3 μm or more, especially preferably 3.5 μm or more, preferably 30 μm or less, more preferably 27 μm or less, and even more preferably 25 μm or less. Such a small 90% cumulative diameter D90 indicates that (C) the inorganic filler does not contain large particles. (B) If the 90% cumulative diameter D90 of the inorganic filler is too small, its distribution is reduced, and backflow may easily occur.

[0076] (B) The ratio of the 50% cumulative diameter D50 to the 90% cumulative diameter D90 of the inorganic filler, D50 / D90, is preferably 0.2 or higher, more preferably 0.3 or higher, especially preferably 0.35 or higher, preferably 0.8 or lower, more preferably 0.7 or lower, and even more preferably 0.65 or lower.

[0077] (B) The difference between the 50% cumulative diameter D50 and the 90% cumulative diameter D90 of the inorganic filler (D90-D50) is preferably 2 μm or more, more preferably 2.5 μm or more, especially preferably 3 μm or more, preferably 20 μm or less, more preferably 18 μm or less, and even more preferably 16 μm or less.

[0078] (B) The 50% cumulative diameter (D50) and 90% cumulative diameter (D90) of the inorganic filler can be determined using laser diffraction based on Mie scattering theory. Specifically, a laser diffraction particle size distribution measuring device can be used to establish the particle size distribution of the (B) inorganic filler on a volume basis. Then, the particle size with a cumulative frequency of 50% from its smallest diameter side (i.e., the median diameter) is set as the 50% cumulative diameter (D50). And, the particle size with a cumulative frequency of 90% from its smallest diameter side is set as the 90% cumulative diameter (D90). The sample for measurement can preferably be prepared by ultrasonically dispersing 100 mg of (B) inorganic filler and 10 g of methyl ethyl ketone in an ampoule for 10 minutes. The sample was measured using a laser diffraction particle size distribution measuring device. The light source wavelength was set to blue and red, and the particle size distribution of the inorganic filler (B) was measured using a flow cell method based on a volume reference. The 50% cumulative diameter D50 and 90% cumulative diameter D90 were calculated from the obtained particle size distribution. An example of a laser diffraction particle size distribution measuring device is the "LA-960" manufactured by Horiba Corporation.

[0079] (B) The specific surface area of ​​the inorganic filler, based on the viewpoint of significantly achieving the intended effects of the present invention, is preferably 1 m² / g or more, more preferably 2 m² / g or more, and particularly preferably 3 m² / g or more. There is no particular upper limit, but it is preferably 60 m² / g or less, 50 m² / g or less, or 40 m² / g or less. The specific surface area can be obtained according to the BET method, using a specific surface area measuring device (Macsorb HM-1210 manufactured by MOUNTECH), by adsorbing nitrogen gas onto the surface of the sample, and calculating the specific surface area using the BET multi-point method.

[0080] Examples of commercially available inorganic fillers (B) include Nippon Steel & Sumitomo Metal Materials Co., Ltd.’s “SP60-05” and “SP507-05”; ADMATECHS Co., Ltd.’s “YC100C”, “YA050C”, “YA050C-MJE”, and “YA010C”; DENKA Co., Ltd.’s “UFP-30”; Tokuyama Co., Ltd.’s “SILFIL NSS-3N”, “SILFIL NSS-4N”, and “SILFIL NSS-5N”; and ADMATECHS Co., Ltd.’s “SC2500SQ”, “SO-C4”, “SO-C2”, and “SO-C1”.

[0081] Based on the viewpoint of improving moisture resistance and dispersibility, (B) inorganic fillers are preferably treated with surface treatment agents. Examples of surface treatment agents include fluorosilane coupling agents, aminosilane coupling agents, epoxysilane coupling agents, mercaptosilane coupling agents, silane coupling agents, alkoxysilanes, organosilazane compounds, titanate coupling agents, etc. Furthermore, a single surface treatment agent can be used alone, or two or more can be used in combination.

[0082] Commercially available surface treatment agents include, for example, "KBM403" (3-glycidoxypropyltrimethoxysilane) manufactured by Shin-Etsu Chemical Industry Co., Ltd., "KBM803" (3-mercaptopropyltrimethoxysilane) manufactured by Shin-Etsu Chemical Industry Co., Ltd., "KBE903" (3-aminopropyltriethoxysilane) manufactured by Shin-Etsu Chemical Industry Co., Ltd., "KBM573" (N-phenyl-3-aminopropyltrimethoxysilane) manufactured by Shin-Etsu Chemical Industry Co., Ltd., "SZ-31" (hexamethyldisilazane) manufactured by Shin-Etsu Chemical Industry Co., Ltd., "KBM103" (phenyltrimethoxysilane) manufactured by Shin-Etsu Chemical Industry Co., Ltd., "KBM-4803" (long-chain epoxy silane coupling agent) manufactured by Shin-Etsu Chemical Industry Co., Ltd., and "KBM-7103" (3,3,3-trifluoropropyltrimethoxysilane) manufactured by Shin-Etsu Chemical Industry Co., Ltd., etc.

[0083] The extent of surface treatment using a surface treatment agent is preferably limited to a specific range, based on the viewpoint of improving the dispersibility of the inorganic filler (B). Specifically, it is preferable to surface treat 100 parts by weight of the inorganic filler (B) with 0.2 to 5 parts by weight of a surface treatment agent, more preferably with 0.2 to 3 parts by weight, and even more preferably with 0.3 to 2 parts by weight.

[0084] The degree of surface treatment using a surface treatment agent can be evaluated by the carbon content per unit surface area of ​​the inorganic filler (B). From the viewpoint of improving the dispersibility of the inorganic filler (B), the carbon content per unit surface area of ​​the inorganic filler (B) is preferably 0.02 mg / m² or more, more preferably 0.1 mg / m² or more, and even more preferably 0.2 mg / m² or more. On the other hand, from the viewpoint of suppressing the increase in melt viscosity of the resin varnish and the melt viscosity of the resin flake layer, it is preferably 1 mg / m² or less, more preferably 0.8 mg / m² or less, and even more preferably 0.5 mg / m² or less.

[0085] The carbon content per unit surface area of ​​(B) inorganic filler can be determined by washing the surface-treated (B) inorganic filler with a solvent (e.g., methyl ethyl ketone (MEK)). Specifically, a sufficient amount of MEK as a solvent is added to the surface-treated (B) inorganic filler, and ultrasonic cleaning is performed at 25°C for 5 minutes. After removing the supernatant and drying the solids, the carbon content per unit surface area of ​​the (B) inorganic filler is determined using a carbon analyzer. For example, the "EMIA-320V" manufactured by Horiba Corporation can be used as the carbon analyzer.

[0086] The content of inorganic filler (B) in the resin composition is not particularly limited, but when the non-volatile component in the resin composition is set to 100% by mass, based on the viewpoint of significantly obtaining the expected effect of the present invention, it is, for example, 0% by mass or more, 1% by mass or more, preferably 10% by mass or more, 20% by mass or more, more preferably 30% by mass or more, 40% by mass or more, even more preferably 50% by mass or more, 60% by mass or more, even more preferably 65% ​​by mass or more, 70% by mass or more, particularly preferably 75% by mass or more, 78% by mass or more, the upper limit is preferably 95% by mass or less, more preferably 92% by mass or less, even more preferably 90% by mass or less, and particularly preferably 89% by mass or less. When the content of inorganic filler (B) is too high, the distribution is reduced, and backflow may easily occur.

[0087] <(C)Silane Coupling Agent> The resin composition of the present invention may also contain (C) silane coupling agent as any component other than (A) and (B).

[0088] Examples of silane coupling agents (C) include, for example, aminosilane coupling agents, epoxysilane coupling agents, mercaptosilane coupling agents, alkoxysilane compounds, organosilazane compounds, titanate coupling agents, etc. Among these, epoxysilane coupling agents containing epoxy groups and mercaptosilane coupling agents containing mercapto groups are preferred. Furthermore, a single silane coupling agent can be used alone, or two or more can be used in combination.

[0089] Commercially available products can be used as (C) silane coupling agents. Examples of commercially available silane coupling agents include Shin-Etsu Chemical Co., Ltd.'s "KBM403" (3-glycidoxypropyltrimethoxysilane), Shin-Etsu Chemical Co., Ltd.'s "KBM803" (3-mercaptopropyltrimethoxysilane), Shin-Etsu Chemical Co., Ltd.'s "KBE903" (3-aminopropyltriethoxysilane), Shin-Etsu Chemical Co., Ltd.'s "KBM573" (N-phenyl-3-aminopropyltrimethoxysilane), and Shin-Etsu Chemical Co., Ltd.'s "SZ-3". 1” (hexamethyldisilazane), Shin-Etsu Chemical Industry Co., Ltd.'s "KBM103" (phenyltrimethoxysilane), Shin-Etsu Chemical Industry Co., Ltd.'s "KBM-4803" (long-chain epoxy silane coupling agent), Shin-Etsu Chemical Industry Co., Ltd.'s "KBM-7103" (3,3,3-trifluoropropyltrimethoxysilane), Shin-Etsu Chemical Industry Co., Ltd.'s "KBM503" (3-methacryloxypropyltrimethoxysilane), Shin-Etsu Chemical Industry Co., Ltd.'s "KBM5783", etc.

[0090] (C) The amount of silane coupling agent is not particularly limited, but when all non-volatile components in the resin composition are set to 100% by mass, for example, it is 0% or more by mass, 0.0001% or more by mass, preferably 0.001% or more by mass, more preferably 0.01% or more by mass, particularly preferably 0.05% or more by mass, preferably 1% or less by mass, more preferably 0.5% or less by mass, and particularly preferably 0.3% or less by mass. When the non-volatile components in the resin composition other than (B) inorganic fillers are set to 100% by mass, for example, it is 0% or more by mass, 0.001% or more by mass, preferably 0.01% or more by mass, more preferably 0.1% or more by mass, particularly preferably 0.5% or more by mass, preferably 10% or less by mass, more preferably 5% or less by mass, and particularly preferably 2% or less by mass.

[0091] <(D) Hardening Accelerator> The resin composition of the present invention may also contain (D) a curing accelerator as any component other than (A) to (C). The (D) curing accelerator has the function of a curing catalyst that promotes the curing of the resin composition.

[0092] Examples of (D) curing accelerators include phosphorus-based curing accelerators, amine-based curing accelerators, imidazole-based curing accelerators, guanidine-based curing accelerators, and metal-based curing accelerators. Among these, imidazole-based curing accelerators are preferred. A single curing accelerator may be used alone, or two or more may be used in combination.

[0093] Examples of phosphorus-based hardening accelerators include triphenylphosphine, phosphonium borate compounds, tetraphenylphosphonium tetraphenylborate, n-butylphosphonium tetraphenylborate, tetrabutylphosphonium decanoate, (4-methylphenyl)triphenylphosphonium thiocyanate, tetraphenylphosphonium thiocyanate, butyltriphenylphosphonium thiocyanate, etc., with triphenylphosphine and tetrabutylphosphonium decanoate being preferred.

[0094] Examples of amine-based hardening accelerators include trialkylamines such as triethylamine and tributylamine, 4-dimethylaminopyridine, benzyldimethylamine, 2,4,6-tris(dimethylaminomethyl)phenol, 1,8-diazabicyclo(5,4,0)-undecene, 1,8-diazabicyclo[5,4,0]-undecene-7,4-dimethylaminopyridine, and 2,4,6-tris(dimethylaminomethyl)phenol, with 4-dimethylaminopyridine and 1,8-diazabicyclo(5,4,0)-undecene being preferred.

[0095] Examples of imidazole-based hardening accelerators include 2-methylimidazolium, 2-undecylimidazolium, 2-heptadecylimidazolium, 1,2-dimethylimidazolium, 2-ethyl-4-methylimidazolium, 1,2-dimethylimidazolium, 2-ethyl-4-methylimidazolium, 2-phenylimidazolium, 2-phenyl-4-methylimidazolium, 1-benzyl-2-methylimidazolium, 1-benzyl-2-phenylimidazolium, 1-cyanoethyl-2-methylimidazolium, 1-cyanoethyl-2-undecylimidazolium, 1-cyanoethyl-2-ethyl-4-methylimidazolium, 1-cyanoethyl-2-phenylimidazolium, 1-cyanoethyl-2-undecylimidazolium trimellitate, 1-cyanoethyl-2-phenylimidazolium trimellitate, 2,4-diamino-6-[2'-methylimidazolyl-(1')]-ethyl-s-triazine ... -[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-phenylimidazolyl isocyanuric acid adduct, 2-phenyl-4,5-dihydroxymethylimidazolium, 2-phenyl-4-methyl-5-hydroxymethylimidazolium, 2,3-dihydro-1H-pyrrolo[1,2-a]benzimidazole, 1-dodecyl-2-methyl-3-benzylimidazolyl chloride, 2-methylimidazoline, 2-phenylimidazoline and other imidazole compounds and adducts of imidazole compounds with epoxy resins, preferably 2-ethyl-4-methylimidazolium and 1-benzyl-2-phenylimidazolium.

[0096] Commercially available imidazole-based hardening accelerators can also be used, such as "P200-H50" manufactured by Mitsubishi Chemical Corporation, and "CUREZOL 2MZ", "2E4MZ", "C11Z", "C11Z-CN", "C11Z-CNS", "C11Z-A", "2MZ-OK", "2MA-OK", "2MA-OK-PW", and "2PHZ" manufactured by Shikoku Chemical Industry Co., Ltd.

[0097] Examples of guanidine-based hardening promoters include dicyandiamide, 1-methylguanidine, 1-ethylguanidine, 1-cyclohexylguanidine, 1-phenylguanidine, 1-(o-tolyl)guanidine, dimethylguanidine, diphenylguanidine, trimethylguanidine, tetramethylguanidine, pentamethylguanidine, 1,5,7-triazabicyclo[4.4.0]dec-5-ene, 7-methyl-1,5,7-triazabicyclo[4.4.0]dec-5-ene, 1-methylbiguanidine, 1-ethylbiguanidine, 1-n-butylbiguanidine, 1-n-octadecylbiguanidine, 1,1-dimethylbiguanidine, 1,1-diethylbiguanidine, 1-cyclohexylbiguanidine, 1-allylbiguanidine, 1-phenylbiguanidine, 1-(o-tolyl)biguanidine, etc.

[0098] Examples of metal-based hardening accelerators include organometallic complexes or organometallic salts of metals such as cobalt, copper, zinc, iron, nickel, manganese, and tin. Specific examples of organometallic complexes include organocobalt complexes such as cobalt(II) and cobalt(III) acetylacetonate, organocopper complexes such as copper(II) acetylacetonate, organozinc complexes such as zinc(II) acetylacetonate, organoiron complexes such as iron(III) acetylacetonate, organonickel complexes such as nickel(II) acetylacetonate, and organomanganese complexes such as manganese(II) acetylacetonate. Examples of organometallic salts include zinc octanoate, tin octanoate, zinc naphthenate, cobalt naphthenate, tin stearate, and zinc stearate.

[0099] The content of (D) curing accelerator in the resin composition is not particularly limited, but when all non-volatile components in the resin composition are set to 100% by mass, for example, it is 0% or more by mass, 0.001% or more by mass, preferably 0.01% or more by mass, more preferably 0.05% or more by mass, particularly preferably 0.1% or more by mass, preferably 5% or less by mass, more preferably 1% or less by mass, and particularly preferably 0.5% or less by mass. When the non-volatile components other than (B) inorganic fillers in the resin composition are set to 100% by mass, for example, it is 0% or more by mass, 0.01% or more by mass, preferably 0.1% or more by mass, more preferably 0.5% or more by mass, particularly preferably 1% or more by mass, preferably 20% or less by mass, more preferably 10% or less by mass, and particularly preferably 5% or less by mass.

[0100] <(E) Free radical polymeric compounds> The resin composition of the present invention may also contain (E) free radical polymerizable compounds as any component other than (A) to (D).

[0101] As (E) radical polymerizable compounds, compounds having vinyl unsaturated bonds are used. Examples of such (E) radical polymerizable compounds are compounds having free radical polymerizable groups such as vinyl, allyl, 1-butenyl, 2-butenyl, acrylyl, methacrylyl, fumaryl, maleyl, vinylphenyl, styryl, cinnamyl, and maleimino (2,5-dihydro-2,5-dioxo-1H-pyrrole-1-yl). One (E) radical polymerizable compound may be used alone or in combination of two or more.

[0102] Specific examples of (E) radical polymerizable compounds include, for example, (meth)acrylic acid-based radical polymerizable compounds having one or more acrylonitrile groups and / or methacrylic acid groups; styrene-based radical polymerizable compounds having one or more vinyl groups directly bonded to aromatic carbon atoms; allyl-based radical polymerizable compounds having one or more allyl groups; and maleimide-based radical polymerizable compounds having one or more maleimide groups. Among these, (meth)acrylic acid-based radical polymerizable compounds are preferred.

[0103] (E) The free radical polymerizable compound preferably contains a polyepoxide structure. By using an (E) free radical polymerizable compound containing a polyepoxide structure, the flexibility of the cured resin composition of the present invention can be improved, the warping of the cured composition can be reduced, or the adhesion between the cured composition and the conductor layer can be improved.

[0104] The structure of the polyepoxide is represented by the formula -(RfO)n-. In this formula, n usually represents an integer of 2 or more. This integer n is preferably 4 or more, more preferably 9 or more, even more preferably 11 or more, usually 101 or less, preferably 90 or less, even more preferably 68 or less, even more preferably 65 or less. In formula (4), Rf independently represents an alkyl group that may have substituents. The aforementioned alkyl group preferably has 1 or more carbon atoms, more preferably 2 or more, more preferably 6 or less, even more preferably 5 or less, even more preferably 4 or less, even more preferably 3 or less, and most preferably 2. Specific examples of polyoxyethylene structures include polyethylene oxide structures, polypropylene oxide structures, polybutane oxide structures, poly(ethylene oxide-copolymer-propylene oxide) structures, poly(ethylene oxide-random-propylene oxide) structures, poly(ethylene oxide-alternating-propylene oxide) structures, and poly(ethylene oxide-block-propylene oxide) structures.

[0105] (E) The number of polyepoxide structures contained in one molecule of the free radical polymerizable compound may be one or more. (E) The number of polyepoxide structures contained in one molecule of the free radical polymerizable compound is preferably two or more, more preferably four or more, even more preferably nine or more, particularly preferably 11 or more, preferably 101 or less, more preferably 90 or less, even more preferably 68 or less, and particularly preferably 65 or less. (E) When one molecule of the free radical polymerizable compound contains two or more polyepoxide structures, these polyepoxide structures may be the same or different from each other.

[0106] Examples of commercially available products containing (E) radical polymerizable compounds with a polyepoxide structure include monofunctional acrylates "AM-90G", "AM-130G", and "AMP-20GY" manufactured by Shin-Nakamura Chemical Industry Co., Ltd.; difunctional acrylates "A-1000", "A-B1206PE", "A-BPE-20", and "A-BPE-30"; monofunctional methacrylates "M-20G", "M-40G", "M-90G", "M-130G", and "M-230G"; and difunctional methacrylates "23G", "BPE-900", "BPE-1300N", and "1206PE". Other examples include "LIGHT ESTER BC", "LIGHT ESTER 041MA", "LIGHT ACRYLATE EC-A", and "LIGHT ACRYLATE EHDG-AT" manufactured by Kyoei Chemical Co., Ltd.; "FA-023M" manufactured by Hitachi Chemical Co., Ltd.; and "BLENMER (registered trademark) PME-4000", "BLENMER (registered trademark) 50POEO-800B", "BLENMER (registered trademark) PLE-200", "BLENMER (registered trademark) PLE-1300", "BLENMER (registered trademark) PSE-1300", "BLENMER (registered trademark) 43PAPE-600B", and "BLENMER (registered trademark) ANP-300" manufactured by Nippon Oil Co., Ltd. Among them, the preferred are "M-130G" having a polyepoxide structure (specifically a polyethylene oxide structure) (n average 13); and "M-230G" having a polyepoxide structure (specifically a polyethylene oxide structure) (n average 23).

[0107] (E) The equivalent amount of vinyl unsaturated bonds in the free radical polymerizable compound is preferably 20 g / eq. to 3000 g / eq., more preferably 50 g / eq. to 2500 g / eq., even more preferably 70 g / eq. to 2000 g / eq., and particularly preferably 90 g / eq. to 1500 g / eq. The equivalent amount of vinyl unsaturated bonds refers to the mass of the free radical polymerizable compound per equivalent of vinyl unsaturated bonds.

[0108] (E) The weight average molecular weight (Mw) of the free radical polymerizable compound is preferably 150 or more, more preferably 250 or more, even more preferably 400 or more, preferably 40,000 or less, even more preferably 10,000 or less, even more preferably 5,000 or less, and particularly preferably 3,000 or less.

[0109] The content of (E) free radical polymerizable compounds in the resin composition is not particularly limited, but when all non-volatile components in the resin composition are set to 100% by mass, the content may be, for example, 0% or more by mass, 0.1% or more by mass, preferably 0.5% or more by mass, more preferably 1% or more by mass, particularly preferably 3% or more by mass, preferably 15% or less by mass, more preferably 10% or less by mass, and particularly preferably 5% or less by mass. When the non-volatile components other than (B) inorganic fillers in the resin composition are set to 100% by mass, the content may be, for example, 0% or more by mass, 1% or more by mass, preferably 5% or more by mass, more preferably 10% or more by mass, particularly preferably 20% or more by mass, preferably 40% or less by mass, more preferably 30% or less by mass, and particularly preferably 25% or less by mass.

[0110] <(F) Free radical polymerization initiators> The resin composition of the present invention may further contain (F) radical polymerization initiator as an optional component. Preferably, the (F) radical polymerization initiator is a thermal polymerization initiator that generates free radicals upon heating. One (F) radical polymerization initiator may be used alone, or two or more may be used in combination.

[0111] Examples of (F) radical polymerization initiators include peroxide-based radical polymerization initiators and azo-based radical polymerization initiators. Peroxide-based radical polymerization initiators are preferred.

[0112] Examples of peroxide-based free radical polymerization initiators include hydrogen peroxide compounds such as 1,1,3,3-tetramethylbutyl hydroperoxide; dialkyl peroxide compounds such as tributyl cumene peroxide, di-tert-butyl peroxide, di-tert-hexyl peroxide, diisopropylbenzene peroxide, 1,4-bis(1-tert-butylperoxy-1-methylethyl)benzene, 2,5-dimethyl-2,5-bis(tert-butylperoxy)hexane, and 2,5-dimethyl-2,5-bis(tert-butylperoxy)-3-hexyne; and dilauryl peroxide, didecyl peroxide, dicyclohexyl peroxide, and bis(4-butylperoxy)-3-hexyne. Diacyl peroxide compounds such as tert-butylcyclohexyl)peroxydicarbonate; peroxide ester compounds such as tert-butylperoxyacetate, tert-butylperoxybenzoate, tert-butylperoxyisopropyl monocarbonate, tert-butylperoxy-2-ethylhexanoate, tert-butylperoxyneodecanate, tert-hexylperoxyisopropyl monocarbonate, tert-butylperoxylaurate, (1,1-dimethylpropyl)2-ethylperoxyhexanoate, tert-butyl-2-ethylperoxyhexanoate, tert-butyl-3,5,5-trimethylperoxyhexanoate, tert-butylperoxy-2-ethylhexyl monocarbonate, and tert-butylperoxymaleic acid.

[0113] Examples of azo radical polymerization initiators include azo nitrile compounds such as 2,2'-azobis(4-methoxy-2,4-dimethylpentanonitrile), 2,2'-azobis(2,4-dimethylpentanonitrile), 2,2'-azobisisobutyronitrile, 2,2'-azobis(2-methylbutyronitrile), 1,1'-azobis(cyclohexane-1-carboxylonitrile), 1-[(1-cyano-1-methylethyl)azo]methoxymethylamine, and 2-phenylazo-4-methoxy-2,4-dimethylpentanonitrile; 2,2'-azobis[2-methyl-N-[1,1-bis(hydroxymethyl)-2-hydroxyethyl]propionylamine], 2,2'-azobis[2-methyl-N-[1,1-bis(hydroxymethyl)-2-hydroxyethyl]propionylamine], 2,2'-azobis[2-methyl-N-[1,1-bis(hydroxymethyl)-2-hydroxyethyl]propionylamine], and 2-phenylazobis[2-methyl-N-[1,1-bis(hydroxymethyl)-2-hydroxyethyl]propionylamine]. Azoamide compounds such as [hydroxymethyl]ethyl[propionic acid], 2,2'-azobis[2-methyl-N-[2-(1-hydroxybutyl)]-propionic acid], 2,2'-azobis[2-methyl-N-(2-hydroxyethyl)-propionic acid], 2,2'-azobis(2-methylpropionic acid) dihydrate, 2,2'-azobis[N-(2-propenyl)-2-methylpropionic acid], 2,2'-azobis(N-butyl-2-methylpropionic acid), 2,2'-azobis(N-cyclohexyl-2-methylpropionic acid); alkyl azo compounds such as 2,2'-azobis(2,4,4-trimethylpentane) and 2,2'-azobis(2-methylpropane).

[0114] (F) The free radical polymerization initiator is preferably one with intermediate temperature activity. Specifically, the 10-hour half-life temperature T10 (°C) of the (F) free radical polymerization initiator preferably falls within a specific low temperature range. The aforementioned 10-hour half-life temperature T10 is preferably 50°C to 110°C, more preferably 50°C to 100°C, and even more preferably 50°C to 80°C. Examples of commercially available (F) free radical polymerization initiators include, for example, "LUPEROX 531M80" manufactured by ARKEMA FUJI, "PERHEXYL (registered trademark) O" manufactured by Nippon Oil Co., Ltd., and "MAIB" manufactured by Fujifilm and Wako Pure Chemical Industries Co., Ltd.

[0115] The content of (F) free radical polymerization initiator in the resin composition is not particularly limited, but when all non-volatile components in the resin composition are set to 100% by mass, it can be, for example, 0% by mass or more, 0.0001% by mass or more, preferably 0.001% by mass or more, more preferably 0.01% by mass or more, particularly preferably 0.05% by mass or more, preferably 1% by mass or less, more preferably 0.5% by mass or less, and particularly preferably 0.1% by mass or less. When the non-volatile components other than (B) inorganic filler in the resin composition are set to 100% by mass, it can be, for example, 0% by mass or more, 0.001% by mass or more, preferably 0.01% by mass or more, more preferably 0.1% by mass or more, particularly preferably 0.3% by mass or more, preferably 3% by mass or less, more preferably 1% by mass or less, and particularly preferably 0.5% by mass or less.

[0116] <(G) Compounds containing a polyether backbone> The resin composition of the present invention may also contain (G) a compound with a polyether backbone as any component other than (A) to (F). (G) A compound with a polyether backbone may be used alone or in combination of two or more.

[0117] (G) Compounds containing a polyether backbone are polymer compounds having a polyether backbone. The polyether backbone of (G) compounds containing a polyether backbone is preferably a polyoxyalkylene backbone composed of one or more monomer units selected from ethylene oxide units and propylene oxide units. Therefore, (G) compounds containing a polyether backbone preferably do not contain a polyether backbone comprising monomer units with 4 or more carbon atoms, such as butylene oxide units or phenylene oxide units.

[0118] (G) Compounds containing a polyether backbone may also contain a silica backbone. Examples of silica backbones include, for example, polydialkylsiloxane backbones such as polydimethylsiloxane backbones; polydiarylsiloxane backbones such as polydiphenylsiloxane backbones; polyalkylarylsiloxane backbones such as polymethylphenylsiloxane backbones; polydialkyl-diarylsiloxane backbones such as polydimethyl-diphenylsiloxane backbones; polydialkyl-alkylarylsiloxane backbones such as polydimethyl-methylphenylsiloxane backbones; and polydiaryl-alkylarylsiloxane backbones such as polydimethyl-methylphenylsiloxane backbones, with polydialkylsiloxane backbones being preferred, and polydimethylsiloxane backbones being particularly preferred. Compounds containing a silicon oxide backbone (G) and a polyether backbone include, for example, polyoxyalkylene-modified silicon oxides and alkyl-etherified polyoxyalkylene-modified silicon oxides (polyoxyalkylene-modified silicon oxides in which at least a portion of the polyether backbone terminal is an alkoxy group). Furthermore, compounds containing a polyether backbone (G) may also contain hydroxyl groups.

[0119] Examples of compounds containing a polyether backbone (G) include linear polyoxyethylene glycols such as polyethylene glycol, polypropylene glycol, and polyoxyethylene polyoxypropylene glycol; polyoxyethylene glycerol ethers, polyoxypropylene glycerol ethers, polyoxyethylene trimethylolpropane ethers, polyoxypropylene trimethylolpropane ethers, polyoxyethylene diglycerol ethers, polyoxypropylene diglycerol ethers, polyoxyethylene pentaerythritol ethers, polyoxypropylene pentaerythritol ethers, polyoxyethylene sorbitol, polyoxypropylene sorbitol, polyoxyethylene polyoxypropylene sorbitol, etc. Polyoxyalkylene glycols such as pear tartrate (polyoxyalkylene glycols) and polyoxyalkylene glycols (polyoxyalkylene glycols); polyoxyethylene monoalkyl ethers, polyoxyethylene dialkyl ethers, polyoxypropylene monoalkyl ethers, polyoxypropylene dialkyl ethers, polyoxyethylene polyoxypropylene monoalkyl ethers, polyoxyethylene polyoxypropylene dialkyl ethers and polyoxyalkylene ethers; polyoxyalkylene esters such as polyoxyethylene monoester, polyoxyethylene diester, polypropylene glycol monoester, polypropylene glycol diester, polyoxyethylene polyoxypropylene monoester, polyoxyethylene polyoxypropylene diester and polyoxyalkylene polyoxypropylene diester (including acetate, propionate, butyrate, (meth)acrylate, etc.); polyoxyethylene monoester, polyoxyethylene diester, polyoxypropylene monoester, polyoxypropylene diester Polyoxyethylene alkyl ether esters, polyoxyethylene polyoxypropylene monoesters, polyoxyethylene polyoxypropylene diesters, polyoxyethylene alkyl ether esters, polyoxypropylene alkyl ether esters, polyoxyethylene polyoxypropylene alkyl ether esters, etc., including alkyl ether esters, propionates, butyrates, (meth)acrylates, etc.; polyoxyethylene alkylamines, polyoxypropylene alkylamines, polyoxyethylene polyoxypropylene alkylamines, etc., including alkyl alkyl alkylamines; polyoxyethylene alkylamines, polyoxypropylene alkylamines, polyoxyethylene polyoxypropylene alkyl alkylamines, etc., including alkyl alkyl alkyl alkylamines; polyoxyethylene dimethylsiloxanes, polyoxypropylene dimethylsiloxanes, polyoxyethylene polyoxypropylene dimethylsiloxanes, polyoxyethylene polydimethylsiloxyalkyl Polyoxyalkyl-modified silica, including dimethylsiloxane, polyoxypropylene polydimethylsiloxyalkyl dimethylsiloxane, polyoxyethylene polyoxypropylene polydimethylsiloxyalkyl dimethylsiloxane, etc.; alkyl etherified polyoxyalkyl-modified silica, including polyoxypropylene alkyl ether dimethylsiloxane, polyoxypropylene alkyl ether dimethylsiloxane, polyoxyethylene polyoxypropylene alkyl ether dimethylsiloxane, polyoxyethylene alkyl ether polydimethylsiloxyalkyl dimethylsiloxane, polyoxypropylene alkyl ether polydimethylsiloxyalkyl dimethylsiloxane, etc. (polyoxyalkyl-modified silica with at least a portion of the polyether backbone terminal being alkoxy).

[0120] (G) The number-average molecular weight of the compound containing the polyether backbone is preferably 500 to 40,000, more preferably 500 to 20,000, and even more preferably 500 to 10,000. The weight-average molecular weight of the compound containing the polyether backbone is preferably 500 to 40,000, more preferably 500 to 20,000, and even more preferably 500 to 10,000. The number-average molecular weight and weight-average molecular weight were determined by gel permeation chromatography (GPC) using values ​​converted to polystyrene.

[0121] (G) The compound containing a polyether backbone is preferably liquid at 25°C. (G) The viscosity of the compound containing a polyether backbone at 25°C is preferably 100,000 mPa·s or less, more preferably 50,000 mPa·s or less, even more preferably 30,000 mPa·s or less, even more preferably 10,000 mPa·s or less, even more preferably 5,000 mPa·s or less, even more preferably 4,000 mPa·s or less, even more preferably 3,000 mPa·s or less, even more preferably 2,000 mPa·s or less, and most preferably 1,500 mPa·s or less. (G) The lower limit of the viscosity of the compound containing a polyether backbone at 25°C is preferably 10 mPa·s or more, more preferably 20 mPa·s or more, even more preferably 30 mPa·s or more, even more preferably 40 mPa·s or more, and most preferably 50 mPa·s or more. Viscosity can be measured using a type B viscometer (mPa·s).

[0122] Examples of commercially available compounds containing a polyether backbone (G) include, for instance, Nippon Oil Co., Ltd.'s "PRONON #102", "PRONON #104", "PRONON #201", "PRONON #202B", "PRONON #204", "PRONON #208", "UNILUBE 70DP-600B", and "UNILUBE 70DP-950B" (polyoxyethylene polyoxypropylene glycol); and ADEKA Co., Ltd.'s "PLURONIC L-23", "PLURONIC L-31", "PLURONIC L-44", "PLURONIC L-61", "ADEKA PLURONIC L-62", "PLURONIC L-64", "PLURONIC L-71", "PLURONIC L-72", "PLURONIC L-101", and "PLURONIC L-72". "PLURONIC 17R-2", "PLURONIC 17R-3", "PLURONIC 17R-4 (Polyoxyethylene Polyoxypropylene Glycol); Shin-Etsu Silicon Oxide Co., Ltd.'s "KF-6011", "KF-6011P", "KF-6012", "KF-6013", "KF-6015", "KF-6016", "KF-6017", "KF-6017P", "KF-6043", "KF-6004", "KF351A", "KF352A", "KF353", "KF35" 4L, KF355A, KF615A, KF945, KF-640, KF-642, KF-643, KF-644, KF-6020, KF-6204, X22-4515, KF-6028, KF-6028P, KF-6038, KF-6048, KF-6025 (polyoxyalkylene modified silica), etc.

[0123] The content of (G) compounds containing a polyether backbone in the resin composition is not particularly limited, but when all non-volatile components in the resin composition are set to 100% by mass, the content may be, for example, 0% or more by mass, 0.001% or more by mass, preferably 0.01% or more by mass, more preferably 0.1% or more by mass, particularly preferably 0.5% or more by mass, preferably 5% or less by mass, more preferably 2% or less by mass, and particularly preferably 1% or less by mass. When the non-volatile components (B) other than inorganic fillers in the resin composition are set to 100% by mass, the content may be, for example, 0% or more by mass, 0.1% or more by mass, preferably 0.5% or more by mass, more preferably 1% or more by mass, particularly preferably 5% or more by mass, preferably 15% or less by mass, more preferably 10% or less by mass, and particularly preferably 7% or less by mass.

[0124] <(H) Other Additives> The resin composition of the present invention may also contain any additives as non-volatile components other than those in (A) to (G) above. Examples of such additives include organic fillers such as rubber particles, polyamide microparticles, and silica particles; thermoplastic resins such as polycarbonate resin, phenoxy resin, polyvinyl acetal resin, polyolefin resin, polyurethane resin, and polyester resin; organometallic compounds such as organocopper compounds, organozinc compounds, and organocobalt compounds; colorants such as phthalocyanine blue, phthalocyanine green, iodine green, diazo yellow, crystal violet, titanium dioxide, and carbon black; polymerization inhibitors such as hydroquinone, catechol, pyrogallol, and phenothiazine; leveling agents such as silica-based leveling agents and acrylic polymer-based leveling agents; tackifiers such as bentonite and montmorillonite; defoamers such as silica-based defoamers, acrylic defoamers, fluorinated defoamers, and vinyl resin-based defoamers; ultraviolet absorbers such as benzotriazole-based ultraviolet absorbers; adhesion enhancers such as urea silane; and triazole-based adhesion promoters. Adhesion enhancers, including tetrazolium-based adhesion enhancers and triazine-based adhesion enhancers; antioxidants, including hindered phenolic antioxidants and hindered amine antioxidants; fluorescent whitening agents, including diphenylethylene derivatives; surfactants, including fluorine-based surfactants; flame retardants, including phosphorus-based flame retardants (e.g., phosphate ester compounds, phosphazene compounds, phosphonic acid compounds, red phosphorus), nitrogen-based flame retardants (e.g., melamine sulfate), halogen-based flame retardants, and inorganic flame retardants (e.g., antimony trioxide); dispersants, including phosphate ester dispersants, polyoxyethylene dispersants, acetylene dispersants, silica dispersants, anionic dispersants, and cationic dispersants; and stabilizers, including borate ester stabilizers, titanate stabilizers, aluminate stabilizers, zirconate stabilizers, isocyanate stabilizers, carboxylic acid stabilizers, and carboxylic anhydride stabilizers. Additives can be used alone or in any combination of two or more.

[0125] <(I) Organic Solvents> The resin composition of the present invention may further contain (I) any organic solvent as a volatile component. (I) One organic solvent may be used alone, or two or more may be used in any proportion. The less solvent, the better. The amount of solvent, relative to 100% by mass of all non-volatile components in the resin composition of the present invention, is preferably 3% by mass or less, more preferably 1% by mass or less, more preferably 0.5% by mass or less, even more preferably 0.1% by mass or less, even more preferably 0.01% by mass or less, and most preferably (0% by mass) is absent.

[0126] <Manufacturing Method of Resin Composition> The resin composition of the present invention can be manufactured, for example, by mixing the above-mentioned components. The components can be mixed partially or entirely simultaneously, or sequentially. During the mixing process, the temperature can be appropriately set, thus allowing for temporary or continuous heating and / or cooling. Furthermore, stirring or agitation can also be performed during the mixing process.

[0127] <Uses of Resin Compositions> The resin composition of the present invention can be suitably used as a resin composition for sealing organic EL devices and semiconductor and other electronic devices (resin composition for sealing), particularly as a resin composition for sealing semiconductors (resin composition for semiconductor sealing), and preferably as a resin composition for sealing semiconductor wafers (resin composition for semiconductor wafer sealing). Furthermore, the resin composition can be used as an insulating layer for insulating purposes other than sealing. For example, the aforementioned resin composition can preferably be used as a resin composition for forming an insulating layer for semiconductor wafer packaging (resin composition for insulating layer of semiconductor wafer packaging) and as a resin composition for forming an insulating layer for circuit boards (including printed wiring boards) (resin composition for insulating layer of circuit board).

[0128] Based on the advantage of utilizing the photosensitive resin composition layer formed on the cured layer of the resin composition of the present invention to improve the resolution, the resin composition of the present invention is preferably used as a sealing layer or insulating layer for forming semiconductor wafer packages. Examples of semiconductor wafer packages include FC-CSP, MIS-BGA package, ETS-BGA package, fan-out WLP (wafer-level package), fan-in WLP, fan-out PLP (planar-level package), and fan-in PLP.

[0129] Furthermore, the aforementioned resin composition can also be used as an underfill material, for example, as a material for MUF (Molding Under Filling) used after a semiconductor wafer is attached to a substrate.

[0130] In addition, the aforementioned resin composition can be used in a wide range of applications, such as sheet-like laminates like resin sheets and prepregs, solder resists, grain adhesives, pore-filling resins, and component embedding resins.

[0131] <Resin Sheets> The resin sheet comprises a support and a resin composition layer disposed on the support. The resin composition layer is formed from the resin composition of the present invention.

[0132] The thickness of the resin composition layer, based on the viewpoint of thinning, is preferably 600 μm or less, more preferably 500 μm or less. The lower limit of the resin composition layer thickness is preferably 1 μm or more, 5 μm or more, more preferably 10 μm or more, even more preferably 50 μm or more, and particularly preferably 100 μm or more.

[0133] Furthermore, the thickness of the cured layer obtained by curing the resin composition layer is preferably 600 μm or less, more preferably 500 μm or less. The lower limit of the thickness of the cured layer is preferably 1 μm or more, 5 μm or more, more preferably 10 μm or more, even more preferably 50 μm or more, and particularly preferably 100 μm or more.

[0134] Examples of supports include films made of plastic materials, metal foils, and release paper, with films and metal foils made of plastic materials being more preferred.

[0135] When a film made of plastic material is used as a support, examples of plastic materials include polyesters such as polyethylene terephthalate (hereinafter sometimes abbreviated as "PET") and polyethylene naphthalate (hereinafter sometimes abbreviated as "PEN"), acrylic polymers such as polycarbonate (hereinafter sometimes abbreviated as "PC") and polymethyl methacrylate (hereinafter sometimes abbreviated as "PMMA"); cyclic polyolefins; triacetyl cellulose (hereinafter sometimes abbreviated as "TAC"); polyether sulfides (hereinafter sometimes abbreviated as "PES"); polyether ketones; polyimides, etc. Among these, polyethylene terephthalate and polyethylene naphthalate are preferred, and inexpensive polyethylene terephthalate is particularly preferred.

[0136] When using metal foil as a support, copper foil, aluminum foil, etc. are preferred. Copper foil is the most preferred. Copper foil can be made of copper alone or as an alloy of copper with other metals (such as tin, chromium, silver, magnesium, nickel, zirconium, silicon, titanium, etc.).

[0137] The support can also be treated with matte finish, corona treatment, antistatic treatment, etc. on the surface that bonds with the resin composition layer.

[0138] Furthermore, as a support, it can also be used in supports with a release layer on the surface bonded to the resin composition layer. Examples of release agents used in the release layer of a support with a release layer include one or more release agents selected from the group consisting of alkyd resins, polyolefin resins, urethane resins, and silicone resins. Examples of commercially available release agents include "SK-1," "AL-5," and "AL-7" manufactured by LINTEC, an alkyd resin-based release agent company. Examples of supports with a release layer include "LUMIRROR T60" manufactured by Toray Industries, Inc.; "PUREX" manufactured by Teijin Corporation; and "UNIPEEL" manufactured by Unitika Corporation.

[0139] The thickness of the support is preferably in the range of 5μm to 75μm, and more preferably in the range of 10μm to 60μm. Furthermore, when using a support with an attached release layer, the overall thickness of the support with the release layer is preferably within the above-mentioned range.

[0140] Resin flakes can be manufactured, for example, by coating the resin composition of the present invention onto a support using a coating apparatus such as a die coater. Alternatively, if necessary, the resin composition of the present invention can be dissolved in an organic solvent to prepare a resin varnish, which is then coated to manufacture resin flakes. By using an organic solvent and adjusting the viscosity, coatability can be improved. When using the resin composition or resin varnish of the present invention containing an organic solvent, the resin composition or resin varnish of the present invention is typically dried after coating to form a resin composition layer of the present invention.

[0141] Examples of organic solvents include ketone solvents such as acetone, methyl ethyl ketone, and cyclohexanone; acetate solvents such as ethyl acetate, butyl acetate, cellolytic acetate, propylene glycol monomethyl ether acetate, and carbitol acetate; carbitol solvents such as cellolytic and butyl carbitol; aromatic hydrocarbon solvents such as toluene and xylene; and acetamide solvents such as dimethylformamide, dimethylacetamide (DMAc), and N-methylpyrrolidone. A single organic solvent can be used, or two or more can be combined in any proportion.

[0142] Drying can be carried out by conventional methods such as heating or hot air blowing. Drying conditions are such that the organic solvent content in the resin composition layer is typically less than 10% by mass, preferably less than 5% by mass. Although the specific conditions vary depending on the boiling point of the organic solvent in the resin composition or resin varnish of the present invention, for example, when using the resin composition or resin varnish of the present invention containing 30% to 60% by mass of organic solvent, a resin composition layer can be formed by drying at 50°C to 150°C for 3 to 10 minutes.

[0143] The resin sheet may also include any layer other than the support and resin composition layer, as needed. For example, a protective film based on the support may be provided on the side of the resin composition layer that is not bonded to the support (i.e., the side opposite to the support). The thickness of the protective film may be, for example, 1 μm to 40 μm. The protective film can inhibit the adhesion of dirt or other contaminants to the surface of the resin composition layer or prevent scratches. When the resin sheet has a protective film, the resin sheet can be used by peeling off the protective film. Furthermore, the resin sheet can be rolled into a roll for storage.

[0144] Resin sheets are preferably used in the manufacture of semiconductor wafer packages to form insulating layers (insulating resin sheets for semiconductor wafer packages). For example, resin sheets can be used to form insulating layers on circuit boards (insulating resin sheets for circuit boards). Examples of packages using such substrates include FC-CSP, MIS-BGA packages, and ETS-BGA packages.

[0145] Furthermore, resin sheets are better suited for sealing semiconductor wafers (resin sheets for sealing semiconductor wafers). Examples of suitable semiconductor wafer packages include, for example, fan-out WLP, fan-in WLP, fan-out PLP, and fan-in PLP.

[0146] Furthermore, resin flakes can be used as MUF materials for attaching semiconductor wafers to substrates.

[0147] In addition, resin sheets can be used in a wide range of other applications requiring high insulation reliability. For example, resin sheets can be appropriately used to form the insulating layer of circuit boards such as printed wiring boards.

[0148] <Circuit substrate> The circuit board comprises a cured resin composition. Typically, the circuit board includes a cured layer formed from the cured resin composition, which functions as an insulating layer or a sealing layer. The circuit board can be manufactured, for example, by a manufacturing method including steps (1) and (2). (1) The step of forming a resin composition layer on a substrate. (2) The step of thermally curing the resin composition layer to form a hardened layer.

[0149] In step (1), a substrate is prepared. Examples of substrates include glass epoxy boards, metal substrates (stainless steel, cold-rolled steel sheet (SPCC), silicon wafers, etc.), polyester substrates, polyimide substrates, BT resin substrates, thermosetting polyphenylene ether substrates, etc. The substrate may have a metal layer, such as copper foil, on its surface as part of the substrate. For example, a substrate with a peelable first metal layer and a second metal layer on both surfaces can be used. When using such a substrate, a conductor layer that functions as a wiring layer is typically formed on the side of the second metal layer opposite to the first metal layer. Examples of materials for the metal layer include copper foil, copper foil with a carrier, and conductor layer materials described later, with copper foil being preferred. An example of a substrate with a metal layer is the "Micro Thin" ultra-thin copper foil with a carrier copper foil manufactured by Mitsui Mining & Metals Corporation.

[0150] Alternatively, a conductor layer may be formed on one or both surfaces of the substrate. In the following description, the component comprising the substrate and the conductor layer formed on the surface of the substrate is sometimes appropriately referred to as a "substrate with a wiring layer". Examples of conductor materials contained in the conductor layer include materials containing one or more metals selected from the group consisting of gold, platinum, palladium, silver, copper, aluminum, cobalt, chromium, zinc, nickel, titanium, tungsten, iron, tin, and indium. Single metals or alloys can be used as conductor materials. Examples of alloys include alloys selected from two or more metals in the aforementioned group (e.g., nickel-chromium alloys, copper-nickel alloys, and copper-titanium alloys). From the viewpoint of the wide applicability, cost, and ease of patterning of conductor layer formation, alloys of chromium, nickel, titanium, aluminum, zinc, gold, palladium, silver, or copper as single metals; and alloys of nickel-chromium alloys, copper-nickel alloys, and copper-titanium alloys as alloys are preferred. The preferred metals are single metals such as chromium, nickel, titanium, aluminum, zinc, gold, palladium, silver, or copper; and nickel-chromium alloys, especially single metals such as copper.

[0151] Conductor layers, for example, can be patterned to function as wiring layers. In this case, the line width (circuit width) / split width (inter-circuit width) ratio of the conductor layer is not particularly limited, but is preferably 20 / 20 μm or less (i.e., a spacing of 40 μm or less), more preferably 10 / 10 μm or less, even more preferably 5 / 5 μm or less, even more preferably 1 / 1 μm or less, and most preferably 0.5 / 0.5 μm or more. The spacing may not be the same throughout the conductor layer. The minimum spacing of the conductor layer may be, for example, 40 μm or less, 36 μm or less, or 30 μm or less.

[0152] The thickness of the conductor layer depends on the design of the substrate, but is preferably 3μm to 35μm, more preferably 5μm to 30μm, even more preferably 10μm to 20μm, and most preferably 15μm to 20μm.

[0153] After preparing the substrate, a resin composition layer is formed on the substrate. When forming a conductor layer on the substrate surface, it is preferable to form the resin composition layer to embed the conductor layer into the resin composition layer.

[0154] The resin composition layer can be formed, for example, by compression molding. In compression molding, a substrate on which the resin composition is distributed using a syringe is placed in a mold, and pressure and heat are applied to the resin composition in the mold as needed to form a resin composition layer on the substrate.

[0155] The specific operation of compression molding can be as follows: An upper mold and a lower mold are prepared as the molds for compression molding. A resin composition is distributed onto a substrate using a syringe. The substrate with the resin composition distributed on it is then mounted onto the lower mold. The upper and lower molds are then fastened together, and heat and pressure are applied to the resin composition to perform compression molding.

[0156] Molding conditions vary depending on the composition of the resin composition, and appropriate conditions are adopted to achieve a good seal. For example, the mold temperature during molding is preferably 70°C or higher, more preferably 80°C or higher, particularly preferably 90°C or higher, preferably 200°C or lower, more preferably 170°C or lower, and particularly preferably 150°C or lower. Furthermore, the pressure applied during molding is preferably 1 MPa or higher, more preferably 3 MPa or higher, particularly preferably 5 MPa or higher, preferably 50 MPa or lower, more preferably 30 MPa or lower, and particularly preferably 20 MPa or lower. The curing time is preferably 1 minute or more, more preferably 2 minutes or more, particularly preferably 3 minutes or more, preferably 60 minutes or lower, more preferably 30 minutes or lower, and particularly preferably 20 minutes or lower. Generally, the mold is removed after the resin composition layer has formed. Mold removal can be performed before or after the resin composition has undergone thermosetting.

[0157] Furthermore, the resin composition layer can be formed, for example, by laminating a resin sheet to a substrate. This lamination is performed, for example, by heating and pressing the resin sheet onto the substrate from the support side, thus attaching the resin composition layer to the substrate. Examples of components for heating and pressing the resin sheet onto the substrate (hereinafter sometimes referred to as "heat-pressing components") include, for example, heated metal plates (SUS mirror plates, etc.) or metal rollers (SUS rollers, etc.). It is also preferable not to directly press the heat-pressing component onto the resin sheet, but rather to press it using an elastic material such as heat-resistant rubber in a manner that allows the resin sheet to fully follow the unevenness of the substrate surface.

[0158] The deposition of the substrate and the resin sheet can be performed, for example, by vacuum lamination. In vacuum lamination, the heating and pressing temperature is preferably in the range of 60°C to 160°C, more preferably in the range of 80°C to 140°C. The heating and pressing pressure is preferably in the range of 0.098 MPa to 1.77 MPa, more preferably in the range of 0.29 MPa to 1.47 MPa. The heating and pressing time is preferably in the range of 20 seconds to 400 seconds, more preferably in the range of 30 seconds to 300 seconds. The deposition can preferably be performed under reduced pressure conditions below 13 hPa.

[0159] After lamination, the laminated resin sheet can also be smoothed under normal pressure (atmospheric pressure), for example, by pressing and heating the bonding member from the side of the support. The pressing conditions for smoothing can be the same as the heating and pressing conditions for lamination described above. Furthermore, lamination and smoothing can also be performed continuously using a vacuum laminator.

[0160] After forming a resin composition layer on the substrate, the resin composition layer is thermo-cured to form a cured layer. The thermo-curing conditions of the resin composition layer vary depending on the type of resin composition, but the curing temperature is usually in the range of 120°C to 240°C (preferably in the range of 150°C to 220°C, more preferably in the range of 170°C to 200°C), and the curing time is in the range of 5 minutes to 120 minutes (preferably in the range of 10 minutes to 100 minutes, more preferably in the range of 15 minutes to 90 minutes).

[0161] Before heat curing the resin composition layer, a preheating treatment at a temperature lower than the curing temperature may be performed on the resin composition layer. For example, before heat curing the resin composition layer, the resin composition layer is usually preheated at a temperature of 50°C or higher but not exceeding 120°C (preferably 60°C or higher but not exceeding 110°C, more preferably 70°C or higher but not exceeding 100°C) for at least 5 minutes (preferably 5 minutes to 150 minutes, more preferably 15 minutes to 120 minutes).

[0162] As described above, a circuit board having a cured layer formed from a resin composition can be manufactured. Furthermore, the method for manufacturing the circuit board may include any steps. For example, when manufacturing a circuit board using resin sheets, the manufacturing method of the circuit board may include a step of peeling off a support from the resin sheet. The support may be peeled off before the resin composition layer is heat-cured, or it may be peeled off after the resin composition layer is heat-cured.

[0163] The manufacturing method of a circuit board may include, for example, a step of grinding the surface of the hardened layer after forming a hardened layer. The grinding method is not particularly limited. Examples of grinding methods include chemical mechanical polishing (CMP) using a chemical mechanical polishing apparatus, mechanical polishing using an abrasive cloth, and planar grinding using a rotating abrasive stone.

[0164] The manufacturing method of the circuit board may include, for example, the step of interlayer bonding of the conductor layers (3), or the step of creating holes in the hardened layer. This allows through-holes, vias, and other holes to be formed in the hardened layer. Examples of methods for forming through-holes include laser irradiation, etching, and mechanical drilling. The size and shape of the through-holes can be appropriately determined according to the production design of the circuit board. Furthermore, step (3) can also involve interlayer bonding by grinding or polishing the hardened layer.

[0165] After forming the through-hole, it is preferable to perform a step to remove the adhesive residue inside the through-hole. This step is sometimes called the adhesive residue removal step. For example, when forming a conductor layer on a hardened layer by plating, a wet adhesive residue removal process can be performed on the through-hole. Furthermore, when forming a conductor layer on a hardened layer by sputtering, a dry adhesive residue removal process such as a plasma treatment process can be performed. In addition, the adhesive residue removal step can also be used to roughen the hardened layer.

[0166] Furthermore, before forming the conductor layer on the hardened layer, the hardened layer can be roughened. This roughening process typically roughens the surface of the hardened layer, including the vias. Both dry and wet roughening processes can be performed. Examples of dry roughening processes include plasma treatment. Examples of wet roughening processes include a method that sequentially performs swelling treatment with a swelling solution, roughening treatment with an oxidizing agent, and neutralization treatment with a neutralizing solution.

[0167] After forming vias, a conductor layer can be formed on the hardened layer. By forming a conductor layer at the location of the via, the newly formed conductor layer is connected to the conductor layer on the substrate surface, achieving interlayer bonding. Methods for forming the conductor layer include, for example, plating, sputtering, and vapor deposition. For example, a suitable method such as semi-additive or fully additive plating can be used to plate the surface of the hardened layer to form a conductor layer with the desired wiring pattern. Furthermore, if the support for the resin sheet is a metal foil, a conductor layer with the desired wiring pattern can be formed using a subtractive method. The material of the conductor layer to be formed can be a single metal or an alloy. Moreover, the conductor layer can have a single-layer structure or a multi-layer structure containing two or more layers of different types of materials.

[0168] This section details an embodiment of forming a conductor layer on a hardened layer. A mask layer is formed on the surface of the hardened layer, and an opening is formed in a portion of the mask layer as a mask pattern. Then, after forming a metal layer by sputtering, the mask layer is removed. This allows the formation of a conductor layer with a desired wiring pattern. The aforementioned mask layer is typically formed from a layer of photosensitive resin composition. Furthermore, the opening in the mask layer is formed by exposing and developing the photosensitive resin composition layer.

[0169] The method for manufacturing a circuit board may include a step (4) of removing the substrate. By removing the substrate, a circuit board having a hardened layer and a conductor layer embedded in the hardened layer is obtained. This step (4) may be performed, for example, when using a substrate having a peelable metal layer.

[0170] Semiconductor wafer packaging Semiconductor wafer packages include cured resin compositions. Examples of such semiconductor wafer packages are as follows.

[0171] The first example of a semiconductor wafer package includes the aforementioned circuit substrate and a semiconductor wafer mounted on the circuit substrate. The semiconductor wafer package can be manufactured by bonding the semiconductor wafer to the circuit substrate.

[0172] The bonding conditions between the circuit board and the semiconductor wafer can be any conditions that allow for the conductive connection of the terminal electrodes of the semiconductor wafer to the circuit wiring of the circuit board. For example, conditions used in flip-chip mounting of semiconductor wafers can be adopted. Furthermore, for example, an insulating adhesive can be used to bond the semiconductor wafer and the circuit board.

[0173] An example of a bonding method is the method of pressing a semiconductor wafer onto a circuit board. As for the pressing conditions, the pressing temperature is usually in the range of 120°C to 240°C (preferably in the range of 130°C to 200°C, and even more preferably in the range of 140°C to 180°C), and the pressing time is usually in the range of 1 second to 60 seconds (preferably in the range of 5 seconds to 30 seconds).

[0174] Another example of a bonding method is the method of reflowing a semiconductor wafer onto a circuit board. The reflow conditions can be in the range of 120°C to 300°C.

[0175] After the semiconductor wafer is bonded to the circuit board, the semiconductor wafer can be filled with a mold bottom filler. The above-mentioned resin composition can be used as the mold bottom filler.

[0176] The second example of a semiconductor wafer package includes a semiconductor wafer and a cured resin composition that seals the semiconductor wafer. In these semiconductor wafer packages, the cured resin composition typically functions as a sealing layer. An example of this second semiconductor wafer package is, for instance, a fan-out type WLP.

[0177] The manufacturing method of these semiconductor wafer packages includes the following steps: (A) Step of temporarily fixing the film on the substrate. (B) The step of temporarily fixing the semiconductor wafer onto the temporary fixing film. (C) The step of forming a sealing layer on a semiconductor wafer. (D) The step of peeling the substrate and temporary fixing film from the semiconductor wafer. (E) The step of forming a rewiring layer on the surface of the stripped substrate and temporary fixing film of the semiconductor wafer. (F) The step of forming a rewiring layer as a conductor layer on the rewiring forming layer, and (G) The step of forming a solder resist layer on the rewiring layer. Furthermore, the aforementioned semiconductor wafer packaging manufacturing method may also include the following steps: (H) The step of cutting multiple semiconductor wafer packages into individual semiconductor wafer packages to achieve monolithicization.

[0178] (Step (A)) Step (A) pertains to the deposition of a temporary fixing film on the substrate. The deposition conditions of the substrate and the temporary fixing film are the same as those of the deposition conditions of the substrate and the resin film in the circuit board manufacturing method.

[0179] Examples of substrates include silicon wafers; glass wafers; glass substrates; metal substrates such as copper, titanium, stainless steel, and cold-rolled steel sheets (SPCC); substrates such as FR-4 substrates, which are made by infiltrating epoxy resin into glass fibers and then undergoing thermosetting treatment; and substrates made of bismaleimide triazine resin such as BT resin.

[0180] Temporary fixation films can be made of any material that can be peeled off from a semiconductor wafer and can temporarily fix the semiconductor wafer. Examples of commercially available products include "REVALPHA" manufactured by Nitto Denko Corporation.

[0181] (Step (B)) Step (B) is the step of temporarily fixing the semiconductor wafer onto the temporary fixing film. Temporary fixing of the semiconductor wafer can be performed using equipment such as a flip-chip bonding machine or a die bonding machine. The layout and number of semiconductor wafers can be appropriately set according to the shape and size of the temporary fixing film, the production quantity of the desired semiconductor wafer package, etc. For example, the semiconductor wafers can be arranged in a matrix of multiple columns and multiple rows and temporarily fixed.

[0182] (Step (C)) Step (C) is the step of forming a sealing layer on the semiconductor wafer. The sealing layer is formed by curing a resin composition. The sealing layer is typically formed by a method comprising the steps of forming a resin composition layer on the semiconductor wafer and thermally curing the resin composition layer to form a cured layer serving as the sealing layer. The resin composition layer on the semiconductor wafer can be formed, for example, by using a semiconductor wafer instead of a substrate, in the same manner as the method for forming a resin composition layer on a substrate described in the aforementioned <Circuit Substrate> section.

[0183] After forming a resin composition layer on a semiconductor wafer, the resin composition layer is thermosetting to obtain a sealing layer covering the semiconductor wafer. This allows the semiconductor wafer to be sealed using the cured resin composition. The thermosetting conditions for the resin composition layer can be the same as those used in the circuit board manufacturing method. Furthermore, before thermosetting the resin composition layer, a preheating treatment at a temperature lower than the curing temperature can be performed. The preheating treatment conditions can be the same as those used in the circuit board manufacturing method.

[0184] (Step (D)) Step (D) is the step of peeling the substrate and the temporary fixing film from the semiconductor wafer. The peeling method is preferably an appropriate method corresponding to the material of the temporary fixing film. Examples of peeling methods include heating, foaming, or expanding the temporary fixing film and then peeling it off. Another example of a peeling method is irradiating the temporary fixing film with ultraviolet light onto the substrate to reduce the adhesion of the temporary fixing film and then peeling it off.

[0185] In methods for heating, foaming, or expanding and peeling off a temporary fixation film, the heating conditions are typically 100°C to 250°C for 1 to 90 seconds or 5 to 15 minutes. In methods for reducing the adhesiveness of a temporary fixation film and peeling it off by irradiating it with ultraviolet light, the irradiation dose is typically 10 mJ / cm² to 1000 mJ / cm².

[0186] As described above, when the substrate and temporary fixing film are peeled off from the semiconductor wafer, the surface of the sealing layer is exposed. The semiconductor wafer packaging manufacturing method may include grinding the exposed surface of the sealing layer. Grinding improves the smoothness of the sealing layer surface. The same grinding method described in the circuit board manufacturing method can be used.

[0187] (Step (E)) Step (E) is the step of forming a rewiring layer as an insulating layer on the substrate of the semiconductor wafer and the surface of the temporary fixing film after peeling. Typically, the rewiring layer is formed on the semiconductor wafer and the sealing layer.

[0188] The material for the rewiring layer can be any insulating material. In the case where a sealing layer is formed by curing a resin composition, the rewiring layer formed on the sealing layer is preferably formed by a photosensitive resin composition.

[0189] After the rewiring layer is formed, vias are typically formed in the rewiring layer to enable interlayer bonding between the semiconductor wafer and the rewiring layer. When the rewiring layer is formed with a photosensitive resin, the method for forming the vias typically involves exposing the surface of the rewiring layer through a mask pattern. Examples of active energy lines include ultraviolet light, visible light, electron beams, and X-rays, with ultraviolet light being particularly preferred. Exposure methods can include, for example, contact exposure, where the mask is tightly adhered to the rewiring layer and exposed, and non-contact exposure, where the mask is not tightly adhered to the rewiring layer and parallel light is used for exposure.

[0190] Since the aforementioned exposure forms a latent image in the rewiring layer, subsequent development removes a portion of the rewiring layer, creating a through-hole that serves as an opening through the rewiring layer. Development can be performed using either wet or dry development. Examples of development methods include immersion, coating, spraying, brushing, and extrusion coating; from a resolution perspective, coating is preferred.

[0191] The shape of the through-hole is not particularly limited, but is generally set to circular (or slightly circular). The top diameter of the through-hole is preferably 50 μm or less, more preferably 30 μm or less, even more preferably 20 μm or less, and most preferably 10 μm or less. Here, the top diameter of the through-hole refers to the opening diameter of the through-hole on the surface of the rewire forming layer.

[0192] (Step (F)) Step (F) is the step of forming a rewiring layer as a conductor layer on the rewiring forming layer. The method of forming the rewiring layer on the rewiring forming layer can be the same as the method of forming a conductor layer on a hardened layer in the manufacturing method of a circuit board. Furthermore, steps (E) and (F) can be repeated, and the rewiring layer and the rewiring forming layer can be stacked alternately (additional layers).

[0193] (Step (G)) Step (G) is the step of forming a solder resist layer on the rewiring layer. The solder resist layer can be made of any insulating material. From the viewpoint of ease of manufacturing semiconductor wafer packaging, photosensitive resin and thermosetting resin are preferred. Furthermore, as a thermosetting resin, a resin composition can be used.

[0194] Furthermore, in step (G), bump machining can also be performed as needed to form bumps. Bump machining can be performed using methods such as solder balls or solder plating. Also, the formation of through-holes during bump machining can be performed in the same way as in step (E).

[0195] (Step (H)) In addition to steps (A) to (G), the manufacturing method of semiconductor wafer packages may also include step (H). Step (H) is the step of cutting a plurality of semiconductor wafer packages into individual semiconductor wafer packages for monolithic fabrication. The method of cutting semiconductor wafer packages into individual semiconductor wafer packages is not particularly limited.

[0196] Semiconductor Devices Semiconductor devices are packaged with semiconductor wafers. Examples of semiconductor devices include various semiconductor devices used in electrical products (such as computers, mobile phones, smartphones, tablet computers, wearable devices, digital cameras, medical devices, and televisions) and vehicles (such as motorcycles, automobiles, trams, ships, and airplanes). [Example]

[0197] The present invention will be specifically described below through examples. The present invention is not limited to these examples. Furthermore, unless otherwise specified, the terms "parts" and "%" in the following description refer to "parts by mass" and "% by mass," respectively. The temperature and pressure conditions, unless otherwise specified, are room temperature (25°C) and atmospheric pressure (1 atm), respectively.

[0198] <Examples 1-9 and Comparative Examples 1-4> The resin composition is prepared by mixing specific amounts of each component as shown in Table 1 below. Details of each component shown in Table 1 are as follows.

[0199] (A-1) Epoxy resin: CELLOXIDE 2021P: An alicyclic epoxy resin with an ester backbone (DAICEL manufactures "CELLOXIDE 2021P", a liquid epoxy resin with an epoxy equivalent of 126 g / eq.). HP4032D: Naphthalene-type epoxy resin (DIC Corporation's "HP4032D", liquid epoxy resin, epoxy equivalent 151g / eq.) EX-991L: An epoxy resin containing an alkoxy backbone (EX-991L manufactured by NAGASE CHEMTEX, a liquid epoxy resin with an epoxy equivalent of 450 g / eq.) EG-280: Epoxy resin containing a chromatic structure (EG-280, manufactured by Osaka Gas Chemical Co., Ltd., is a liquid epoxy resin with an epoxy equivalent of 460 g / eq.) YX7400: A resin containing polyvinyl alkylene oxide structure (Mitsubishi Chemical Corporation "YX7400", liquid epoxy resin, epoxy equivalent 440 g / eq.) EP-3950L: Glycidylamine type epoxy resin (EP-3950L manufactured by ADEKA, liquid epoxy resin, epoxy equivalent 95g / eq.) EP-3980S: Glycidylamine type epoxy resin (EP-3980S manufactured by ADEKA, liquid epoxy resin, epoxy equivalent 115g / eq.) EP-4088S: Dicyclopentadiene type epoxy resin (EP-4088S manufactured by ADEKA, liquid epoxy resin, epoxy equivalent 170g / eq.) ZX1059: A 1:1 (mass ratio) mixture of bisphenol A type epoxy resin and bisphenol F type epoxy resin (ZX1059, manufactured by Nippon Steel Chemicals & Materials Co., Ltd., liquid epoxy resin, epoxy equivalent 169 g / eq.) JP-100: An epoxy resin with a butadiene structure (JP-100, manufactured by Nippon Soda Co., Ltd., is a liquid epoxy resin with an epoxy equivalent of 210 g / eq.).

[0200] (A-2) Epoxy Curing Agent: 2,2-Dialenylbisphenol A: A phenolic curing agent (manufactured by SIGMA ALDRICH, active group (phenolic hydroxyl group) equivalent 154 g / eq.) KAYAHARD AA: Amine-based hardener (4,4'-diamino-3,3'-diethyldiphenylmethane, manufactured by Nippon Kayaku Co., Ltd., "KAYAHARD AA", active group (amine group) equivalent 64 g / eq.) MH-700: Anhydride-based hardener (MH-700 manufactured by Shin Nippon Rikka Co., Ltd., active group (anhydride group) equivalent 164g / eq. (1 equivalent of an anhydride group (-COOCO-) is equivalent to 2 equivalents of active group))

[0201] (B) Inorganic fillers: Silicon oxide A: Silicon oxide particles (50% cumulative diameter D50=1.5μm, D90=3.5μm, specific surface area 2.78m² / g, surface treated with KBM573 (Shin-Etsu Chemical Industry Co., Ltd.) Silicon oxide B: Silicon oxide particles (50% cumulative diameter D50=4μm, D90=12μm, specific surface area 3.01m² / g, surface treated with KBM573 (Shin-Etsu Chemical Industry Co., Ltd.)

[0202] (C) Silane coupling agent: KBM-803: (Shin-Etsu Chemical Industry Co., Ltd. manufactures "KBM803", 3-mercaptopropyltrimethoxysilane) KBM-403: (Shin-Etsu Chemical Co., Ltd. manufactures "KBM403", 3-glycidoxypropyltrimethoxysilane)

[0203] (D) Hardening accelerator: 2E4MZ: Imidazole-based hardening promoter (2E4MZ manufactured by Shikoku Chemical Industry Co., Ltd.) 2MA-OK-PW: Imidazole-based hardening accelerator (manufactured by Shikoku Chemical Co., Ltd., "2MA-OK-PW")

[0204] (E) Free radical polymerizable compounds: M-130G: A compound with a methacrylic group and a polyethylene oxide structure (M-130G manufactured by Shin-Nakamura Chemical Industry Co., Ltd., methacrylic equivalent: 628 g / eq.) M-230G: A compound with a methacrylic group and a polyethylene oxide structure (M-230G manufactured by Shin-Nakamura Chemical Industry Co., Ltd., methacrylic equivalent: 1068 g / eq.)

[0205] (F) Free radical polymerization initiator: PERHEXYL O: Free radical polymerization initiator (manufactured by Nippon Oil Company, "PERHEXYL (registered trademark) O")

[0206] (G) Compounds containing a polyester backbone: Polyether polyol A: A resin synthesized as follows. 22.6 g of ε-caprolactone monomer (DAICEL's "PLAXEL M"), 10 g of polypropylene glycol, diol type, 3,000 (manufactured by Fujifilm and Kaku Pure Chemicals Co., Ltd.), and 1.62 g of tin(II) 2-ethylhexanoate (manufactured by Fujifilm and Kaku Pure Chemicals Co., Ltd.) were fed into a reaction vessel. The mixture was heated to 130°C under nitrogen atmosphere and stirred for approximately 16 hours. The product was dissolved in chloroform, reprecipitated with methanol, and dried to obtain polyester polyol resin A with hydroxyl-terminated aliphatic backbone. GPC analysis showed Mn = 9000. L-64: Polyoxyethylene polyoxypropylene glycol (L-64 manufactured by ADEKA Corporation) KF-6012: Polyoxyalkylene modified silicone resin (Shin-Etsu Chemical Co., Ltd. "KF-6012", viscosity (25℃): 1500 mm² / s)

[0207] <Experimental Example 1: Viscosity Measurement> The viscosity of the resin composition of the examples or comparative examples was determined using an E-type viscometer RE-80U (manufactured by Toki Sangyo Co., Ltd.) calibrated with a JS52000 viscosity-calibrated standard solution and a 3°×R9.7 conical rotor at a temperature of 25°C and a rotation speed of 1 rpm.

[0208] <Experimental Example 2: Evaluation of Distribution, Dispensing Performance, and Resin Flowability> Prepare a 12oz syringe (SAN EI TECH 5194C, rear end cap A605, front end cap 5192RT, plunger 5196PRS, syringe outlet inner diameter 14.22mm, outer diameter 19.30mm, opening inner diameter 40.26mm, length from outlet to opening 311.40mm) filled with 200g of the resin composition obtained in the examples or comparative examples (room temperature (23°C)). Install a nozzle (the tube is made of silicone, the syringe connector is made of polypropylene, the tube is 52mm long, the length of the tube protruding from the syringe connector is 25mm, the syringe connector is 52mm long, the nozzle outlet (tube side) outer diameter 12mm, inner diameter 9mm, nozzle opening (syringe connector side) outer diameter 14.22mm) and install the syringe on a distributor (APIC YAMADA "manual liquid distributor"). The height (distance perpendicular to the face of the silicon wafer) from the surface of a horizontally positioned 12-inch silicon wafer (Ra 10Å or less) to the nozzle outlet is set to 3 cm. From the nozzle outlet, 40 g ± 1.5 g of resin composition is distributed on the 12-inch silicon wafer at room temperature (23°C) at a rate of 2 g / s. Distribution is stopped at the point when 40 g ± 1.5 g is distributed, forming a resin dome of the resin composition.

[0209] Evaluation of distribution: If backflow of resin composition leaks from the plunger side during distribution, it is marked as "×"; if it does not occur, it is marked as "○".

[0210] Evaluation of dispensing performance: Due to poor separation between the resin composition and the liquid at the nozzle outlet, if the dispensing stops and the distributed resin composition remains connected, or if resin drips from the nozzle outlet after the dispensing is completed, it is marked as "×". If none of these occur, it is marked as "○".

[0211] Resin flowability evaluation: After distribution, under conditions of 120℃ and 6MPa, molding is performed using a compression mold device. When the resin can be molded without any unfilled parts in the mold, it is marked as "○"; when the resin leaks from the mold and contaminates the device, it is marked as "×".

[0212] <Experimental Example 3: Calculation of H2 / H1 and L1 / L2 values> Prepare a 12oz syringe (SAN EI TECH 5194C, rear end cap A605, front end cap 5192RT, plunger 5196PRS, syringe nozzle inner diameter 14.22mm, outer diameter 19.30mm, opening inner diameter 40.26mm, length from nozzle to opening 311.40mm) filled with 200g of the resin composition obtained in the example or comparative example (room temperature (23°C)). Without installing the nozzle, install the syringe on the dispenser (APIC YAMADA "manual liquid dispenser"). The height (distance perpendicular to the surface of the silicon wafer) from the surface of a horizontally positioned 12-inch silicon wafer (Ra 10 Å or less) to the nozzle outlet is set to 5 cm. From the nozzle outlet, 40 g ± 1.5 g of resin composition is distributed onto the 12-inch silicon wafer at room temperature (23°C) at a rate of 2 g / s. Distribution stops at 40 g ± 1.5 g, forming a resin dome. In Comparative Example 3, since the nozzle is in contact with the resin dome when distribution stops, the nozzle is pulled up and removed from the resin dome after distribution stops.

[0213] After the resin dome is formed, the shape change of the resin dome is observed at room temperature (23℃). The height H1 of the resin dome from the contact surface with the silicon wafer to the top of the resin dome is measured 60 seconds after the distribution is completed, the diameter L1 of the contact surface between the resin dome and the silicon wafer, the height H2 of the resin dome from the contact surface with the silicon wafer to the top of the resin dome 180 seconds after the distribution is completed, and the diameter L2 of the contact surface between the resin dome and the silicon wafer are calculated. The values ​​of H2 / H1 and L1 / L2 are calculated. When the following formulas (1) and (2) are satisfied, the evaluation is "○" and when they are not satisfied, the evaluation is "×".

[0214] Furthermore, in the embodiments and comparative examples other than Comparative Example 3, the point at which the resin composition is distributed to 40g ± 1.5g is defined as the point at which the distribution is completed. In Comparative Example 3, the point at which the dispensing nozzle moves away from the resin dome after the operation of pulling the nozzle away from the resin dome is defined as the point at which the distribution is completed. .

[0215] The content of non-volatile components in the resin compositions of the examples and comparative examples, the test results and evaluation results are shown in Table 1 below.

[0216]

[0217] As shown in Table 1, when condition (1) is met, the distribution, dispensing operation and resin flow properties are good.

[0218] 10: Syringe filled with resin composition 11: Syringe 12: Resin composition 13: Plunger 14: Female thread section 15: Spit out 16: Opening 17: Front cover 18: Rear end cover 20: Nozzle 21: Management Department 22: Syringe connection part 23: Nozzle ejection section 24: Nozzle opening 25: Male thread section 30: Resin Dome 40: Silicon wafers

Claims

1. A syringe filled with a resin composition, comprising a syringe and a resin composition filled within the syringe, the resin composition comprising (A-1) epoxy resin and (B) inorganic filler, wherein the 90% cumulative diameter D90 of the inorganic filler (B) is 30 μm or less, and the difference (D90-D50) between the 90% cumulative diameter D90 and the 50% cumulative diameter D50 is 20 μm or less; when the non-volatile components in the resin composition are set to 100% by mass, the content of the inorganic filler (B) is 65% by mass or more and 95% by mass or less; when the non-volatile components in the resin composition other than the inorganic filler (B) are set to 100% by mass, the content of the epoxy resin (A-1) is 10% by mass or more and 90% by mass or less; the resin composition further comprises (I) an organic solvent, wherein the organic solvent (I) is 1% by mass or less relative to all non-volatile components in the resin composition (100% by mass). The resin composition is distributed on the surface of a horizontally set silicon wafer to form a resin dome. In the evaluation test of the resin composition to measure the shape change of the resin dome, the height of the resin dome from the contact surface with the silicon wafer to the top of the resin dome 60 seconds after the distribution is completed is set as H1, and the height of the resin dome from the contact surface with the silicon wafer to the top of the resin dome 180 seconds after the distribution is completed is set as H2. The following condition (1) is satisfied.

2. The syringe filled with resin composition as claimed in claim 1, wherein the aforementioned evaluation test includes distributing 40g ± 1.5g of 23°C resin composition at a speed of 2g / s on the surface of the silicon wafer from a dispensing port located at a height of 5cm above the surface of the silicon wafer, at a temperature of 23°C, and stopping the distribution to form a resin dome of the resin composition.

3. As in claim 2, for a syringe filled with resin composition, in the aforementioned evaluation test, when the distribution of the resin composition stops and the nozzle is not in contact with the resin dome, the point at which 40g ± 1.5g of resin composition is distributed is taken as the aforementioned distribution completion point. When the distribution of the resin composition stops and the nozzle is in contact with the resin dome, after the distribution stops, the nozzle is pulled up to perform an operation to pull the nozzle away from the resin dome, and the point at which the nozzle leaves the resin dome is taken as the aforementioned distribution completion point.

4. As in the syringe filled with resin composition in claim 1, wherein the diameter of the contact surface between the resin dome and the silicon wafer 60 seconds after the distribution is completed is set as L1, and the diameter of the contact surface between the resin dome and the silicon wafer 180 seconds after the distribution is completed is set as L2, then the following condition (2) is satisfied.

5. The syringe filled with the resin composition as requested in item 1, wherein the viscosity of the resin composition, as measured using a type E viscometer at a temperature of 25°C and a rotation speed of 1 rpm, is less than 1000 Pa‧s.

6. The syringe filled with the resin composition as requested in item 1, wherein the viscosity of the resin composition, as measured using a type E viscometer at a temperature of 25°C and a rotation speed of 1 rpm, is 100 Pa·s or more and 500 Pa·s or less.

7. The syringe filled with a resin composition as claimed in claim 1, wherein the resin composition contains (C) a silane coupling agent.

8. A resin composition is distributed on the surface of a horizontally positioned silicon wafer to form a resin dome. In an evaluation test of the resin composition to measure the shape change of the resin dome, H1 is defined as the height from the contact surface between the resin dome and the silicon wafer to the top of the resin dome 60 seconds after the distribution is completed, and H2 is defined as the height from the contact surface between the resin dome and the silicon wafer to the top of the resin dome 180 seconds after the distribution is completed. The following condition (1) is satisfied: the resin composition includes (A-1) epoxy resin and (B) inorganic filler, the 90% cumulative diameter D90 of (B) inorganic filler is 30 μm or less, and the difference between the 90% cumulative diameter D90 and the 50% cumulative diameter D50 (D90-D50) is 20 μm or less. When the non-volatile components in the resin composition are set to 100% by mass, the content of (B) inorganic filler is 65% to 95% by mass. When the non-volatile components other than (B) inorganic filler in the resin composition are set to 100% by mass, the content of (A-1) epoxy resin is 10% to 90% by mass. The resin composition further contains (I) organic solvent, and relative to 100% by mass of all non-volatile components in the resin composition, (I) organic solvent is 1% by mass or less.

9. The resin composition as claimed in claim 8, wherein the aforementioned evaluation test includes distributing 40g ± 1.5g of the 23°C resin composition on the surface of the silicon wafer from an outlet located at a height of 5cm above the surface of the silicon wafer, at a rate of 2g / second under 23°C conditions, and stopping the distribution to form a resin dome of the resin composition.

10. The resin composition as claimed in claim 9, wherein in the aforementioned evaluation test, when the distribution of the resin composition stops and the nozzle is not in contact with the resin dome, the point at which 40g ± 1.5g of the resin composition is distributed is taken as the aforementioned distribution completion point; when the distribution of the resin composition stops and the nozzle is in contact with the resin dome, the nozzle is pulled up after the distribution stops, and the nozzle is pulled away from the resin dome, and the point at which the nozzle leaves the resin dome is taken as the aforementioned distribution completion point.

11. As in the resin composition of claim 8, wherein the diameter of the contact surface between the resin dome and the silicon wafer 60 seconds after the distribution is completed is set as L1, and the diameter of the contact surface between the resin dome and the silicon wafer 180 seconds after the distribution is completed is set as L2, then the following condition (2) is satisfied.

12. The resin composition of claim 8, wherein the viscosity of the resin composition, as measured using a type E viscometer at a temperature of 25°C and a rotation speed of 1 rpm, is less than 1000 Pa‧s.

13. The resin composition of claim 8, wherein the viscosity of the resin composition, as measured using a type E viscometer at a temperature of 25°C and a rotation speed of 1 rpm, is 100 Pa·s or more and 500 Pa·s or less.

14. The resin composition of claim 8, wherein the resin composition comprises (C) a silane coupling agent.

15. The resin composition of claim 8 is used to form an insulating layer for semiconductor wafer packaging.

16. The resin composition of claim 8 is used to form an insulating layer of a circuit board.

17. The resin composition of claim 8 is used to seal a semiconductor wafer package.

18. A cured form of a resin composition as claimed in any one of claims 8 to 17.

19. A circuit board comprising an insulating layer formed by a cured resin composition of any one of claims 8 to 17.

20. A semiconductor wafer package comprising a circuit board as claimed in claim 19 and a semiconductor wafer mounted on the circuit board.

21. A semiconductor device comprising a semiconductor wafer package as claimed in claim 20.

22. A semiconductor wafer package comprising a hardened resin composition of any one of claims 8 to 17, which seals the semiconductor wafer.

23. A semiconductor device comprising a semiconductor wafer package as claimed in claim 22.

24. An evaluation method for a resin composition, wherein a resin composition is distributed on the surface of a horizontally positioned silicon wafer to form a resin dome, and the shape change of the resin dome is measured. The method is characterized by defining the height from the contact surface between the resin dome and the silicon wafer to the top of the resin dome 60 seconds after the distribution is completed as H1, and defining the height from the contact surface between the resin dome and the silicon wafer to the top of the resin dome 180 seconds after the distribution is completed as H2, and determining whether the following condition (1) is satisfied.

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