Resin composition, liquid sealing agent, underfill material, method for producing sealing material, and electronic device

Abstract

To provide a resin composition that has low coefficient of thermal expansion after curing, has low hygroscopicity, and is low in viscosity.SOLUTION: A resin composition comprises a zeolite, an inorganic filler other than zeolite, and a resin, wherein the zeolite has a weight loss rate of 1% or more at 800°C based on the weight at 400°C, as determined by thermogravimetric analysis (TGA), when the temperature thereof is raised to 800°C at the temperature increase rate of 10°C / min in the air atmosphere and held at 800°C for 10 minutes.SELECTED DRAWING: None

Description

Technical Field

[0001] The present invention relates to a resin composition, a liquid encapsulant, an underfill material, a method for manufacturing an encapsulant, and an electronic device.

Background Art

[0002] The liquid encapsulant used as an underfill material is required to be excellent in injectability, adhesiveness, curability, storage stability, etc., and to generate no voids. Further, the portion encapsulated with the liquid encapsulant is required to be excellent in moisture resistance, thermal cycle resistance, reflow resistance, crack resistance, warpage resistance, etc. In order to satisfy the above requirements, as the liquid encapsulant used as an underfill material, those having an epoxy resin as a main component are widely used.

[0003] Further, in order to improve the moisture resistance and thermal cycle resistance, particularly the thermal cycle resistance, of the portion encapsulated with the liquid encapsulant, a filler made of an inorganic substance such as a silica filler (hereinafter sometimes referred to as "inorganic filler") is used in the liquid encapsulant. By doing so, it is known to control the difference in the coefficient of thermal expansion between a substrate made of an organic material such as an epoxy resin and a semiconductor element, and to reinforce the bump electrodes (see Patent Document 1).

Prior Art Documents

Patent Documents

[0004]

Patent Document 1

Summary of the Invention

Problems to be Solved by the Invention

[0005] Liquid encapsulants (resin compositions) using inorganic fillers such as silica fillers do not have a sufficiently low coefficient of thermal expansion, and from the perspective of thermal cycle resistance and the like, it is required to further lower the coefficient of thermal expansion. Further, zeolite is known as an inorganic filler having a low coefficient of thermal expansion, but a liquid composition containing zeolite tends to have a high viscosity, and when used as an underfill material, the injectability (gap infiltration property) decreases. Therefore, it is difficult to obtain a liquid encapsulant with good injectability while lowering the coefficient of thermal expansion of the cured product.

[0006] Further, although zeolite is known to have high hygroscopicity, the presence of water may reduce the dielectric constant and reliability of electronic materials. Therefore, the material used for this application is required to have low hygroscopicity.

[0007] Therefore, an object of the present invention is to provide a resin composition having a low coefficient of thermal expansion after curing, low hygroscopicity, and low viscosity.

Means for Solving the Problems

[0008] As a result of intensive studies on the above problems, the present inventors have found that the above problems can be solved by using a resin composition having a specific configuration, and have completed the present invention. The gist of the present invention is as follows. [1] A resin composition containing zeolite, an inorganic filler other than zeolite, and a resin, wherein the zeolite has a weight loss rate at 800 ° C. based on the weight at 400 ° C. of 1% or more when heated to 800 ° C. at a heating rate of 10 ° C. / min in an air atmosphere and held at 800 ° C. for 10 minutes by thermogravimetric analysis (TGA). [2] The resin composition according to [1] above, wherein the zeolite has d6r as CBU. [3] The resin composition according to [1] or [2] above, wherein the zeolite contains a zeolite having a structure of an oxygen 8-membered ring or less. [4] The resin composition according to any one of [1] to [3] above, wherein the zeolite contains a zeolite having a CHA-type structure. [5] The resin composition according to any one of [1] to [4] above, wherein the sphericity of the zeolite is 0.7 or more. [6] The resin composition according to any one of [1] to [5] above, wherein the roundness of the zeolite is 0.800 or more. [7] The resin composition according to any one of [1] to [6] above, wherein the zeolite is an aluminosilicate. [8] The resin composition according to any one of [1] to [7] above, wherein the inorganic filler other than the zeolite is silica. [9] The resin composition according to any one of [1] to [8] above, wherein the average particle diameter of the inorganic filler other than the zeolite is 0.1 to 5 μm.

[10] The resin composition according to any one of [1] to [9] above, wherein the mass ratio of the zeolite to the inorganic filler other than the zeolite is 5 / 65 to 40 / 30.

[11] The resin composition according to any one of [1] to

[10] above, wherein the content of the inorganic filler other than the zeolite is 1 to 50% by mass.

[12] The resin composition according to any one of [1] to

[11] above, wherein the resin contains a thermosetting resin.

[13] The resin composition according to

[12] above, wherein the thermosetting resin contains an epoxy resin.

[14] A liquid encapsulant comprising the resin composition according to any one of [1] to

[13] above.

[15] An underfill material comprising the resin composition according to any one of [1] to

[13] above.

[16] A method for producing a sealing material, comprising a step of filling a gap with the resin composition according to any one of [1] to

[13] above and then curing it.

[17] An electronic device comprising the sealing material obtained by the production method according to

[16] above. [Effect of the Invention]

[0009] According to the present invention, it is possible to provide a resin composition having a low coefficient of thermal expansion after curing, low moisture absorption, and low viscosity. [Embodiments for Carrying Out the Invention]

[0010] [Resin composition] The resin composition of the present invention (hereinafter sometimes referred to as "the present resin composition") contains zeolite, an inorganic filler other than zeolite, and a resin. The present resin composition is preferably liquid at room temperature. When the present resin composition is liquid at room temperature (hereinafter sometimes referred to as "liquid composition"), it is preferably used as a liquid encapsulant, and is particularly suitable as an underfill material. Hereinafter, each component will be described in detail. When it is assumed that the resin composition is liquid at room temperature, the resin composition shall be read as a liquid composition. In this specification, "liquid at room temperature" means having fluidity between 10°C and 35°C.

[0011] [Zeolite]< Zeolites generally refer to a group of crystalline substances composed of a three-dimensional network structure containing silicon or aluminum and oxygen, and having pores derived from the skeletal structure. Such characteristic structures are applied to adsorbents and catalysts. Therefore, organic substances such as organic structure-directing agents incorporated into the pores during the synthesis of zeolites generally cause pore blockage and reduce the adsorption and catalytic abilities of zeolites, and are thus usually removed by firing or the like. However, the zeolite used in the present resin composition (hereinafter sometimes referred to as "the present zeolite") is characterized by containing an organic substance, preferably a component derived from an organic structure-directing agent which is a raw material of the zeolite, inside the pores. Examples of the method for producing a zeolite containing an organic substance, preferably a component derived from an organic structure-directing agent, inside the pores include, but are not limited to, not performing or partially performing the usual firing treatment during the production process of the zeolite. Specific examples of the characteristics of a zeolite containing an organic substance, preferably a component derived from an organic structure-directing agent, inside the pores include that, when heated to 800 °C at a heating rate of 10 °C / min in an air atmosphere and held at 800 °C for 10 minutes by thermogravimetric analysis (TGA), the weight loss rate at 800 °C is 1% or more based on the weight at 400 °C. In the heat treatment in the high temperature range from 400 °C to 800 °C, the adsorbed water and organic substances, preferably the organic structure-directing agent, present in the pores of the zeolite desorb, and thus the value of the weight loss rate is considered to be larger than that of a normally fired zeolite (hereinafter sometimes referred to as "fired zeolite"). By using zeolite containing an organic substance, preferably a component derived from an organic structure-directing agent, inside such pores, the cured product of this resin composition exhibits low moisture absorption. The mechanism by which such zeolite exhibits low moisture absorption is speculated as follows. Zeolite exhibits adsorptivity to water and other substances because zeolite has a porous structure and acid sites that are adsorption sites. It is presumed that the presence of an organic substance, preferably a component derived from an organic structure-directing agent, in the pores does not allow for a complete porous structure, resulting in a decrease in the adsorptivity to water and other substances and a decrease in moisture absorption. From the above perspective, when this zeolite is heated to 800 °C at a heating rate of 10 °C / min in an air atmosphere and held at 800 °C for 10 minutes by thermogravimetric analysis (TGA), the weight loss rate at 800 °C based on the weight at 400 °C (hereinafter, may be simply referred to as "weight loss rate") is 1% or more, preferably 2% or more, and more preferably 3% or more. The weight loss rate may be 5% or more, 10% or more, or 20% or more. Regarding the upper limit value, there is no particular limitation as long as the effects of the present invention are achieved. For example, it may be 50% or less.

[0012] (Particle size of zeolite) The particle size of this zeolite is preferably 5.0 μm or less. When the particle size of the zeolite is 5.0 μm or less, the resin composition can be sufficiently filled even in a narrow gap. From the above perspective, the smaller the particle size of this zeolite, the more preferable it is, and the lower limit is not particularly limited. In addition, when the particle size of the zeolite is small, there is also an advantage that it is easily mixed uniformly with other components such as resin. Specifically, the particle size of this zeolite is more preferably less than 5.0 μm, even more preferably 4.5 μm or less, and particularly preferably 4.0 μm or less.

[0013] On the other hand, regarding the lower limit value, there is no particular limitation. However, from the perspective of easy handling and the difficulty of increasing the viscosity of this resin composition, it may be 0.05 μm or more, 0.1 μm or more, 0.3 μm or more, 0.5 μm or more, or 1.0 μm or more. The particle size of this zeolite shall mean the diameter of the circle (equivalent circle diameter) with the largest diameter having an area equal to the projected area of the particle in the observation of the particles by a scanning electron microscope (SEM). Further, this zeolite may have a plurality of zeolite particles aggregated to form secondary particles, but in this case, the particle size of the zeolite is the particle size of the primary particles.

[0014] When using zeolite, usually, zeolite particles are not used alone but as a plurality of zeolite particle groups. That is, in one aspect of the present invention, it is preferable to use it as a zeolite group containing at least the zeolite particles of the present invention. In one aspect composed of such a plurality of zeolite particles, the average primary particle size of the zeolite is preferably in the range of 0.05 μm or more and 5.0 μm or less, more preferably 0.1 μm or more and 4.0 μm or less, and even more preferably 0.5 μm or more and 3.5 μm or less. The average primary particle size of the zeolite is determined by randomly selecting 50 zeolites (particles in a powder or liquid composition), measuring their particle sizes, and taking the average value.

[0015] (Structure of Zeolite) Zeolite is a compound composed of silicon or aluminum and oxygen, with a TO 4 unit (the T element is an element other than oxygen that constitutes the framework) as the basic unit. Specifically, zeolites include crystalline porous aluminosilicates (aluminosilicates), crystalline porous aluminophosphates (ALPOs), or crystalline porous silicoaluminophosphates (SAPOs), etc. This zeolite may have any of the above structures, but aluminosilicates are preferred. Zeolite is composed of TO 4 units connected together in several (several to dozens), a structural unit called a Composite Building Unit (hereinafter sometimes referred to as "CBU"). Therefore, it has regular channels (tubular pores) and cavities (voids). Regarding the crystal structures of this CBU and the zeolite described later, they can be represented by the codes that define the zeolite structures determined by the International Zeolite Association (IZA). Note that the zeolite structure can be identified based on the X-ray diffraction pattern obtained by an X-ray structure analyzer (for example, the desktop X-ray diffractometer D2PHASER manufactured by BRUKER) using the 2018 version of the Zeolite Structure Database (http: / / www.iza-structure.org / databases / ).

[0016] (Zeolite framework) The framework of this zeolite preferably has d6r as a CBU. By having d6r, a resin composition with a low coefficient of thermal expansion after curing can be easily obtained. Examples of zeolites having d6r as a CBU include zeolites of AEI, AFT, AFV, AFX, AVL, CHA, EAB, EMT, ERI, FAU, GME, JSR, KFI, LEV, LTL, LTN, MOZ, MSO, MWW, OFF, SAS, SAT, SAV, SBS, SBT, SFW, SSF, SZR, TSC, and -WEN type structures, etc. Among these, from the perspective that water molecules are less likely to penetrate into the pores, zeolites with a structure of 8-membered oxygen ring or less are particularly preferred. Zeolites with a structure of 8-membered oxygen ring or less include zeolites of AEI, AFT, AFX, CHA, ERI, KFI, SAT, SAV, SFW, and TSC type structures, etc. Among these, zeolites of AEI, AFX, CHA, and ERI type structures are particularly preferred because the structure is stable even with shape control, and zeolites having a CHA type structure are most preferred. In this specification, the structure having an 8-membered oxygen ring means a structure in which the number of oxygen elements is 8 when the number of oxygen elements is the largest among the pores composed of oxygen and T elements (elements other than oxygen that constitute the framework) that form the zeolite framework. Also, the above zeolite may be used alone or in combination of two or more types.

[0017] (Average coefficient of thermal expansion of zeolite) The average coefficient of thermal expansion of the zeolite is preferably low because it is easy to slightly reduce the average coefficient of thermal expansion of the liquid composition. Also, it is preferable that the amount of zeolite is small because various physical properties of the resin are less likely to change due to the addition of the zeolite. In particular, it is also preferable that the viscosity increase of the liquid composition can be suppressed. Specifically, the average coefficient of thermal expansion of the zeolite is usually less than 0 ppm / K, preferably -2 ppm / K or less, more preferably -3 ppm / K or less, still more preferably -4 ppm / K or less, and particularly preferably -5 ppm / K or less.

[0018] On the other hand, considering the use as a liquid composition, the average coefficient of thermal expansion of the zeolite is preferably high in that the difference from the average coefficient of thermal expansion of the resin is small and it is difficult for the zeolite and the resin to separate. Therefore, the average coefficient of thermal expansion of the zeolite is usually -1000 ppm / K or more, preferably -900 ppm / K or more, more preferably -800 ppm / K or more, still more preferably -700 ppm / K or more, particularly preferably -500 ppm / K or more, and most preferably -300 ppm / K or more. And in particular, when used for sealing material applications, it is preferably high. Specifically, it is usually -100 ppm / K or more, preferably -50 ppm / K or more, more preferably -40 ppm / K or more, still more preferably -30 ppm / K or more, particularly preferably -25 ppm / K or more, and most preferably -20 ppm / K or more. The average coefficient of thermal expansion of the zeolite can be measured by calculating the lattice constant using an X-ray diffractometer "D8 ADVANCE" manufactured by BRUKER and X-ray diffraction analysis software "JADE". Here, in order to exclude the influence of moisture desorption, the zeolite is usually measured in a dried state. The measurement of the average thermal expansion coefficient of zeolite is usually carried out in the range of 50 to 100 °C. That is, it is a numerical value representing the displacement of the lattice constant per degree Celsius from the average lattice constant at 50 °C and the average lattice constant at 100 °C when the zeolite is heated. Here, the average lattice constant at each temperature is the average value of the lattice constants of the a-axis, b-axis, and c-axis. Note that the measurement of the average thermal expansion coefficient is carried out by gradually heating after waiting until the lattice constant becomes stable.

[0019] Resins generally tend to have a large thermal expansion coefficient in the high-temperature range. Therefore, the average thermal expansion coefficient of zeolite is preferably low, especially when heated up to the high-temperature range. Specifically, the average thermal expansion coefficient (high-temperature range) in the range of 50 to 350 °C is preferably -5 ppm / K or less, more preferably -5.5 ppm / K or less, and even more preferably -6 ppm / K or less. Here, the average thermal expansion coefficient (high-temperature range) of zeolite is a numerical value representing the displacement of the lattice constant per degree Celsius from the average lattice constant at 50 °C and the average lattice constant at 350 °C when the zeolite is heated.

[0020] (Shape of zeolite) This zeolite is preferably spherical. By the zeolite having a spherical shape, an increase in the viscosity of the resin composition containing the zeolite can be suppressed. Specifically, it is preferably to have the following sphericity and roundness.

[0021] <<Sphericity>> The sphericity of this zeolite is preferably 0.7 or more, more preferably 0.8 or more. Also, the upper limit of the sphericity is not particularly limited and may be 1 or less. Note that the sphericity in the case of a cube, which is common in zeolites, is 0.58. Also, in this specification, "sphericity" is the average value of 10 particles obtained by a scanning electron microscope (SEM). In this specification, "sphericity" is defined as "the ratio of the minimum diameter to the maximum diameter of the particle". The maximum diameter and the minimum diameter can be determined by observation with a scanning electron microscope (SEM), respectively.

[0022] <<Circularity>> The circularity of this zeolite is preferably 0.800 or more, more preferably 0.810 or more, still more preferably 0.820 or more, particularly preferably 0.830 or more, and most preferably 0.840 or more. Further, the upper limit of the circularity is not particularly limited and may be 1 or less. Incidentally, the circularity in the case of a cube, which is common in zeolites, is 0.785. In this specification, "circularity" is defined as "4 × π × area / (circumference)" 2 ". The area and the circumference can be determined by observation with a scanning electron microscope (SEM), respectively. In this specification, "circularity" is the average value of 10 particles obtained by a scanning electron microscope (SEM).

[0023] (Framework density of zeolite) The framework density of this zeolite is not particularly limited as long as the effects of the present invention are not impaired. The framework density of zeolite is preferably low in that the structural vibration of zeolite is likely to occur and the average coefficient of thermal expansion is likely to be low. Therefore, the framework density of zeolite is preferably 17.0 T / 1000 Å 3 or less, more preferably 16.0 T / 1000 Å 3 or less. On the other hand, the framework density of zeolite is preferably high in that the structural stability of zeolite is likely to be high. The framework density of zeolite is preferably 12.0 T / 1000 Å 3 or more, more preferably 13.0 T / 1000 Å 3 or more, still more preferably 14.0 T / 1000 Å 3 or more. When the framework density is within the above range, the zeolite can be used as a stable filler. Incidentally, the framework density indicates the number of T atoms present per unit volume of zeolite and is a value determined by the structure of zeolite. In this specification, the numerical values described in the IZA Zeolite Structure Database 2017 Edition (http: / / www.iza-structure.org / databases / ) may be used.

[0024] The framework density is greater than 16.0 T / 1000 Å and less than 17.0 T / 1000 Å 3 and less than 17.0 T / 1000 Å 3 Examples of the following zeolites include zeolites with ERI, LTL, LTN, MOZ, OFF, SAT, SSF, and -WEN type structures. The framework density is greater than 15.0 T / 1000 Å 3 and less than 16.0 T / 1000 Å 3 Examples of the following zeolites include zeolites with AEI, AFT, AFV, AFX, AVL, EAB, GME, LEV, MWW, and SFW type structures. The framework density is greater than 14.0 T / 1000 Å 3 and less than 15.0 T / 1000 Å 3 Examples of the following zeolites include zeolites with CHA, KFI, SAS, and SAV type structures. The framework density is greater than or equal to 14.0 T / 1000 Å 3 Examples of zeolites existing in the following ranges include zeolites with EMT, FAU, JSR, SBS, SBT, and TSC type structures.

[0025] (Composition of Zeolite) The composition of the present zeolite is not particularly limited as long as the effects of the present invention are not impaired. However, since it is advantageous for application to filler uses, aluminosilicates containing at least aluminum atoms and silicon atoms in the framework structure are preferred. Zeolites may be used alone or in any combination and ratio of two or more types.

[0026] In addition, when elements such as gallium, iron, boron, titanium, zirconium, tin, zinc, and phosphorus are used instead of silicon and aluminum, the molar ratio of the oxide of the substituted element may be converted to the molar ratio of alumina or silica. Specifically, when gallium is used instead of aluminum, the molar ratio of gallium oxide may be converted to the molar ratio of alumina.

[0027] (Silica / alumina molar ratio (SAR) of zeolite) The silica / alumina molar ratio of this zeolite (hereinafter sometimes referred to as "SAR", "Si / Al 2 molar ratio", or "Si / Al 2 ratio") is not particularly limited as long as the effects of the present invention are not impaired. The SAR (Si / Al 2 ratio) of the zeolite is preferably high in that the moisture resistance of the cured product is increased and the amount of counter cations can be easily controlled. Therefore, the SAR (Si / Al 2 ratio) of the zeolite is usually 2 or more, preferably 5 or more, more preferably 10 or more, still more preferably 14 or more, particularly preferably 18 or more, particularly preferably 20 or more, particularly preferably 22 or more, particularly preferably 23 or more, particularly preferably 23.5 or more, particularly preferably 24 or more, particularly preferably 24.5 or more, and most preferably 25 or more. On the other hand, the SAR (Si / Al 2 ratio) of the zeolite is preferably low in that it is easily manufactured at low cost. Therefore, the SAR (Si / Al 2 ratio) of the zeolite is usually 2000 or less, preferably 1000 or less, more preferably 500 or less, still more preferably 100 or less, particularly preferably 50 or less, particularly preferably 47.5 or less, particularly preferably 45 or less, particularly preferably 42.5 or less, particularly preferably 40 or less, particularly preferably 39 or less, particularly preferably 38 or less, particularly preferably 37 or less, particularly preferably 36 or less, and most preferably 35 or less. When the Si / Al 2 ratio is within the above range, the amount of counter cations can be easily controlled, and the production cost of the zeolite can also be reduced. The Si / Al 2 ratio of the zeolite can be adjusted by the types and ratios of the silicon-containing compound and the aluminum-containing compound as raw materials, the types and amounts of the structure-directing agents, the use of seed crystals, and the synthesis conditions such as temperature and time.

[0028] (Counter cation of zeolite) The counter cations of the zeolite are not particularly limited as long as the effects of the present invention are not impaired. The counter cations of the zeolite are usually components derived from an organic structure directing agent, protons, alkali metal ions, or alkaline earth metal ions. Preferably, they are components derived from an organic structure directing agent, protons, or alkali metal ions. More preferably, they are components derived from an organic structure directing agent, protons, Li ions, Na ions, or K ions. Even more preferably, they are components derived from an organic structure directing agent. In the case of alkali metal ions or alkaline earth metal ions, the smaller their size, the more preferable it is because the zeolite is more likely to exhibit an average thermal expansion coefficient of less than 0 ppm / K. In the case of a component derived from an organic structure directing agent, it is preferable because the zeolite is more likely to exhibit an average thermal expansion coefficient of less than 0 ppm / K due to its flexibility compared to alkali metal ions and alkaline earth metal ions. That is, as the zeolite, preferably, it is a component type derived from an organic structure directing agent (hereinafter, may be referred to as "as-made"), a proton type, or an alkali metal type. More preferably, it is as-made, a proton type, an Li type, a Na type, or a K type. Even more preferably, it is as-made.

[0029] (Crystallinity of zeolite) The crystallinity of the zeolite is not particularly limited as long as the effects of the present invention are not impaired. The reason is that it is presumed that the Composite Building Unit (CBU) has a greater influence on the average thermal expansion coefficient of the cured product than the structure defined by the IZA code. The crystallinity of the zeolite can be determined by comparing the X-ray diffraction peak of the zeolite with a certain X-ray diffraction peak determined by an X-ray diffractometer (for example, a desktop X-ray diffractometer D2PHASER manufactured by BRUKER). As a specific calculation example, the crystallinity of the LTA-type zeolite in Scientific Reports 2016, 6, Article number: 29210 can be cited.

[0030] (Surface treatment of zeolite) This zeolite may be subjected to surface treatments such as silylation treatment and fluorination treatment as long as the effects of the present invention are not impaired. The surface treatment may be a physical treatment or a chemical treatment.

[0031] (Content of zeolite) From the viewpoint of suppressing the increase in viscosity of the resin composition and lowering the coefficient of thermal expansion, the content of this zeolite in the resin composition is preferably 40% by mass or more and 70% by mass or less, more preferably 45% by mass or more and 65% by mass or less, and even more preferably 50% by mass or more and 60% by mass or less with respect to the total amount of the resin composition.

[0032] <Inorganic filler other than zeolite> This resin composition contains an inorganic filler other than this zeolite (hereinafter, may be referred to as "other inorganic filler"). The other inorganic filler is not particularly limited as long as the effects of the present invention are not impaired, and examples thereof include at least one selected from the group consisting of metals, carbon, metal carbides, metal oxides, and metal nitrides. Examples of metals include silver, copper, aluminum, gold, nickel, iron, and titanium. Examples of carbon include carbon black, carbon fiber, graphite, fullerene, diamond, etc. Examples of metal carbides include silicon carbide, titanium carbide, tungsten carbide, etc. Examples of metal oxides include magnesium oxide, aluminum oxide (alumina), silicon oxides such as silica, calcium oxide, zinc oxide, yttrium oxide, zirconium oxide, cerium oxide, ytterbium oxide, sialon (ceramics composed of silicon, aluminum, oxygen, and nitrogen), etc. Examples of metal nitrides include boron nitride, aluminum nitride, silicon nitride, etc. Among these inorganic fillers, silica is preferable from the viewpoint of being able to reduce the viscosity of the resin composition.

[0033] The average particle diameter of other inorganic fillers is not particularly limited as long as it is within the range in which the effects of the present invention can be achieved, but it is preferably in the range of 0.1 μm or more and 5 μm or less. When it is at least the above lower limit value, the resin composition can have a lower viscosity, and when it is at most the above upper limit value, the filling property into a narrow gap becomes good. From the above viewpoints, the average particle diameter of other inorganic fillers is more preferably in the range of 0.2 μm or more and 4 μm or less, and even more preferably in the range of 0.5 μm or more and 2 μm or less.

[0034] In the present invention, one feature is that zeolite and an inorganic filler other than zeolite are used in combination, and by using them in combination, it is possible to achieve both low CTE and low viscosity. The mass ratio of the inorganic filler other than zeolite to zeolite is not particularly limited as long as it is within the range in which the effects of the present invention can be achieved, but it is preferably in the range of 5 / 65 to 40 / 30. When it is within this range, it is easy to obtain the above effects. From the above points, the mass ratio is more preferably in the range of 10 / 60 to 35 / 35.

[0035] When the present resin composition contains an inorganic filler other than the present zeolite, the content of the other inorganic filler in the present resin composition is preferably in the range of 1% by mass or more and 50% by mass or less, more preferably in the range of 5% by mass or more and 40% by mass or less, and even more preferably in the range of 10% by mass or more and 35% by mass or less. When it is at least the above lower limit value, a reduction in the viscosity of the liquid composition can be achieved, and when it is at most the above upper limit value, the content ratio of the present zeolite is sufficiently high, and the CTE can be reduced.

[0036] The content of the present zeolite in all the inorganic fillers is preferably 50% by mass or more, more preferably 60% by mass or more, and even more preferably 70% by mass or more from the viewpoint that the effects of the present zeolite, that is, low CTE, can be sufficiently exhibited.

[0037] <Total amount of inorganic fillers> The total content of all inorganic fillers (total inorganic fillers) contained in the present resin composition is preferably large in terms of the easy manifestation of the effects as a filler. On the other hand, when the present resin composition is liquid, it is preferably small in terms of high fluidity and easy filling into a narrow space. Specifically, the total content of the total inorganic fillers is preferably 30% by mass or more, more preferably 35% by mass or more, and even more preferably 40% by mass or more with respect to the total amount of the resin composition. On the other hand, it is preferably 95% by mass or less, more preferably 90% by mass or less, and even more preferably 85% by mass or less.

[0038] <Dispersant> The present resin composition may contain a dispersant in order to enhance the dispersibility of inorganic fillers such as the present zeolite. The dispersant contained in the liquid composition containing a resin and a filler is mainly added to the liquid composition containing a resin and a filler having a large polarity difference, thereby improving the interfacial state between the two and improving the compatibility. Thereby, effects such as viscosity reduction, improvement of filler dispersibility, prevention of filler aggregation and sedimentation can be exhibited.

[0039] Examples of the dispersant include acrylic dispersants and polymer dispersants. Here, the "polymer dispersant" means a dispersant having a weight average molecular weight of 1,000 or more. The dispersant is preferably a polymer dispersant. Further, the main chain skeleton of the polymer dispersant is not particularly limited, and examples thereof include a polyurethane skeleton, a polyacrylic skeleton, a polyester skeleton, a polyamide skeleton, a polyimide skeleton, and a polyurea skeleton. From the viewpoint of storage stability, a polyurethane skeleton, a polyacrylic skeleton, and a polyester skeleton are preferable. Further, the structure of the polymer dispersant is not particularly limited, and examples thereof include a random structure, a block structure, a comb structure, and a star structure. Similarly, from the viewpoint of storage stability, a block structure or a comb structure is preferable. Further, the dispersant is preferably a solvent-free type dispersant, particularly a solvent-free type polymer dispersant. By the dispersant not containing a solvent, it is possible to prevent the dispersant from volatilizing and voids from occurring when the resin composition is heat-cured. Commercially available products can be used as the dispersant. Examples of commercially available products include the following dispersants, and among these, a dispersant having at least one of the functional groups of an amino group and an amine salt may be used.

[0040] As commercially available products of polymer dispersants, there are DISPERBYK series wetting dispersants 101, 102, 103, 106, 108, 109, 110, 111, 112, 116, 130, 140, 142, 145, 161, 162, 163, 164, 166, 167, 168, 170, 171, 174, 108, 182, 183, 184, 185, 2000, 2001, 2008, 2020, 2050, 2070, 2096, 2150, 2152, 2155, commercially available from BYK Chemie; EFKA series 4008, 4009, 4010, 4015, 4020, 4046, 4047, 4050, 4055, 4060, 4080, 4300, 4330, 4340, 4400, 4401, 4402, 4403, 4406, 4800, 5010, 5044, 5054, 5055, 5063, 5064, 5065, 5066, 5070, 5244, commercially available from BASF Japan; Solsperse series 3000, 5000, 11200, 13240, 13650, 13940, 16000, 17000, 18000, 20000, 21000, 24000SC, 24000GR, 26000, 28000, 31845, 32000, 32500, 32550, 32600, 33000, 34750, 35100, 35200, 36000, 36600, 37500, 38500, 39000, 53095, 54000, 55000, 56000, 71000, commercially available from Lubrizol; DISPARLON series 1210, 1220, 1831, 1850, 1860, 2100, 2150, 2200, 7004, KS-260, KS-273N, KS-860, KS-873N, PW-36, DN-900, DA-234, DA-325, DA-375, DA-550, DA-1200, DA-1401, DA-7301, commercially available from Nippon Kayaku Co., Ltd.; Ajisper series PB-711, PB-821, PB-822, PN-411, PA-111, commercially available from Ajinomoto Co., Inc.; Surfynol series 104A, 104C, 104E, 104H, 104S, 104BC, 104DPM, 104PA, 104PG-50, 420, 440, DF110D, DF110L, DF37, DF58, DF75, DF210, CT111, CT121, commercially available from Air ProductsCT131, CT136, GA, TG, TGE, STG of the olefin series commercially available from Nissin Chemical Industry Co., Ltd., E1004, 70, 2120, 2190 of the SN sparse series manufactured by San Nopco Ltd., Adeka Cole and Adeka Tol series commercially available from ADEKA Corporation, Sun Nonic series, Naroa Acty CL series, Emalmin series, Newpole PE series, Ionet M series, Ionet D series, Ionet S series, Ionet T series, Sun Separator 100, etc. can be mentioned.

[0041] The content of the dispersant is preferably large in terms of facilitating the uniform dispersion of the inorganic filler in the liquid composition. On the other hand, the content of the dispersant is preferably small in terms of making it difficult for the thermal expansion coefficient to increase due to phase separation between the inorganic filler and resins such as epoxy resins. Therefore, since it is easy to fill the liquid composition into a narrow space and it is easy to obtain a low thermal expansion coefficient after curing, the content of the dispersant is preferably 0.1% by mass or more and 30% by mass or less, more preferably 0.1% by mass or more and 25% by mass or less, based on the total amount of the resin composition.

[0042] <Method for producing zeolite> Known methods can be applied to the method for producing zeolite. For example, when producing CHA-type zeolite, it can be produced with reference to the method described in JP-A-2009-097856. More specifically, an aluminum atom raw material, a silica atom raw material, an organic structure-directing agent, etc. are mixed to prepare an aqueous gel. The mixing order is usually to mix the aluminum atom raw material with water, and then mix the silica atom raw material and the organic structure-directing agent thereto. Next, the prepared aqueous gel is hydrothermally synthesized, the product is separated, and components derived from the attached raw materials are removed by methods such as washing with water and drying to obtain zeolite.

[0043] The particularly preferred zeolite described above can be produced by the following method (hereinafter sometimes referred to as "this production method"). This manufacturing method has a step of hydrothermally synthesizing a raw material composition containing a silicon atom raw material, an aluminum atom raw material, an organic structure-directing agent, and water. Further, in this manufacturing method, as described above, the usual firing treatment is not performed, or when the zeolite after the firing treatment achieves a weight loss rate of 1% or more, it is preferable to perform partial firing. When performing partial firing, the firing conditions described below are preferable. In this manufacturing method, although partial firing can be performed as described above, it is preferable not to perform the firing treatment. That is, this zeolite is preferably not fired (unfired). By not performing the firing treatment, it is easy to achieve a weight loss rate of 1% or more, and thus, it is possible to easily manufacture a zeolite for obtaining a resin composition having a low coefficient of thermal expansion, low hygroscopicity, and low viscosity after curing. If necessary, a desired zeolite (hereinafter, may be referred to as "seed zeolite") may be used.

[0044] <<Silicon atom raw material>> The silicon atom raw material used in the present invention is not particularly limited, and various known substances can be used. For example, colloidal silica, amorphous silica, sodium silicate, trimethylethoxysilane, tetraethyl orthosilicate, aluminosilicate gel, and zeolite can be used. These may be used alone or in combination of two or more in any combination and ratio.

[0045] <<Aluminum atom raw material>> It is preferable to use a water-soluble raw material as the aluminum atom raw material. Further, aluminum hydroxide is preferable in that it has a low alkali metal content.

[0046] <<Organic substance>> This zeolite contains an organic substance inside the pores as described above. As the organic substance, as long as the effects of the present invention are not impaired, it is not particularly limited, and examples include amines, amino acids, fatty acids, surfactants, polymers, organic structure-directing agents, etc. Examples of amines include trimethylamine, adamantylamine, morpholine, etc. Examples of amino acids include lysine, arginine, ornithine. Examples of fatty acids include oleic acid, stearic acid. Examples of surfactants include sodium oleate, sodium stearate. Examples of polymers include polyethylene glycol, polyethyleneimine. Examples of organic structure-directing agents include those described later, etc. Among them, the organic structure-directing agent is preferable because it fills the space inside the zeolite framework, inhibits the diffusion of water vapor inside the pores, and reduces the hygroscopicity. That is, it is preferable that this zeolite contains a component derived from an organic structure-directing agent as the organic substance. When using an organic substance, one type may be used alone, or two or more types may be used in combination at an arbitrary combination and ratio.

[0047] <<Organic Structure-Directing Agent>> As the organic structure-directing agent, various known substances such as tetramethylammonium hydroxide (TMAOH), tetraethylammonium hydroxide (TEAOH), tetrapropylammonium hydroxide (TPAOH), N,N,N-trimethyl-1-adamantylammonium hydroxide (TMAdaOH) can be used. Among these, from the viewpoint of easily retaining the organic substance inside the pores of the zeolite in the range from room temperature to 200 °C and being able to reduce the hygroscopicity of the zeolite, N,N,N-trimethyl-1-adamantylammonium hydroxide (TMAdaOH) is preferable. Also, these may be used alone, or two or more types may be used in combination at an arbitrary combination and ratio. The usage amount of the organic structure-directing agent is usually 0.01 or more, preferably 0.02 or more, more preferably 0.03 or more, still more preferably 0.04 or more, and particularly preferably 0.05 or more in terms of the molar ratio to silicon (Si) contained in the raw material composition. On the other hand, it is usually 1 or less, preferably 0.6 or less, more preferably 0.55 or less, still more preferably 0.5 or less, particularly preferably 0.45 or less, and most preferably 0.4 or less. By using it within this range, it is considered that high-purity spherical zeolite with few by-products is likely to grow.

[0048] <<Water>> From the viewpoint of easy crystal formation, when using the seed crystal zeolite described later, the usage amount of water is usually 5 or more, preferably 7 or more, more preferably 9 or more, still more preferably 10 or more in terms of the molar ratio to silicon (Si) contained in the raw material composition other than the seed crystal zeolite. By setting it within this range, crystal formation is easy and preferable. Also, when hydrothermally synthesizing zeolite under the condition of increasing the amount of water to dilute the raw material concentration, zeolite with a large particle size is likely to be obtained. Further, from the viewpoint of easily obtaining a cost reduction effect for waste liquid treatment, it is usually 50 or less, preferably 40 or less, more preferably 30 or less, still more preferably 25 or less in terms of the molar ratio to silicon (Si).

[0049] <<Alkali metal atom raw material>> For the production of zeolite, an alkali metal atom raw material may be used. The alkali metal atom in the case of using an alkali metal atom raw material is not particularly limited, and known ones used in the synthesis of zeolite can be used, but at least one kind of alkali metal selected from the group consisting of lithium, sodium, potassium, rubidium, and cesium is preferable. Note that a plurality of kinds of alkali metal atoms may be used.

[0050] <<Seed crystal zeolite>> In this production method, zeolite serving as a seed crystal may be used. When using seed crystal zeolite, one kind may be used alone, or two or more kinds may be used in combination at an arbitrary combination and ratio.

[0051] <<Mixing of Raw Materials (Preparation of Reaction-Previous Raw Material Composition)>> The raw material composition can usually be obtained by mixing a silicon atom raw material, an aluminum atom raw material, an organic structure-directing agent, and water, and adding seed zeolite if used. In the production of zeolite, in addition to the above-mentioned components, components such as an acid component for accelerating the reaction and a metal stabilizer such as polyamine may be added in an arbitrary step as necessary.

[0052] <<Aging>> The raw material composition prepared as described above may be hydrothermally synthesized immediately after preparation. However, in order to obtain zeolite having higher crystallinity, it is preferable to age for a certain period of time under predetermined temperature conditions. Particularly when scaling up the reaction, since the stirrability is improved and the raw materials are easily made into a more uniform state, it is preferable to age while stirring the raw materials for a certain period. The temperature for aging is usually 100 °C or lower, preferably 95 °C or lower, more preferably 90 °C or lower. The lower limit is not particularly limited, but the temperature for aging is usually 0 °C or higher, preferably 10 °C or higher. The aging temperature may be constant during aging, or may be changed stepwise or continuously. The aging time is not particularly limited, but is usually 2 hours or longer, preferably 3 hours or longer, more preferably 5 hours or longer. On the other hand, it is usually 30 days or shorter, preferably 10 days or shorter, more preferably 4 days or shorter.

[0053] <<Hydrothermal Synthesis>> Next, the obtained raw material composition is hydrothermally synthesized. Hydrothermal synthesis is usually carried out by putting the raw material composition prepared as described above or the aqueous gel obtained by aging it into a pressure-resistant container, and maintaining a predetermined temperature under self-generated pressure or gas pressurization to such an extent that crystallization is not inhibited, with stirring, or while rotating or rocking the container, or in a static state. The reaction temperature during hydrothermal synthesis is usually 120 °C or higher, preferably 130 °C or higher, more preferably 140 °C or higher, and even more preferably 150 °C or higher, in order to increase the reaction rate. On the other hand, it is usually 230 °C or lower, preferably 220 °C or lower, more preferably 200 °C or lower, and even more preferably 190 °C or lower. The reaction time is not particularly limited, but it is usually 2 hours or longer, preferably 3 hours or longer, more preferably 5 hours or longer. On the other hand, it is usually 30 days or shorter, preferably 10 days or shorter, more preferably 7 days or shorter, and even more preferably 5 days or shorter. The reaction temperature may be constant during the reaction, or may be changed stepwise or continuously.

[0054] <<Drying Process>> After hydrothermal synthesis, the zeolite is separated from the composition after hydrothermal synthesis (hydrothermal synthesis reaction solution). The separation method is not particularly limited, but it is usually separated by filtration, decantation, or direct drying after washing with water. Even when separated by filtration or decantation, it is usually dried thereafter. The drying conditions are not particularly limited. For example, the drying temperature is preferably 50 °C or higher and 200 °C or lower, and more preferably 70 °C or higher and 150 °C or lower. The atmosphere during drying is not particularly limited, and it may be carried out in air or in an inert gas atmosphere such as nitrogen or argon.

[0055] <<Firing>> The dried zeolite may be fired or the like in order to remove the organic structure-directing agent and the like used during production at an arbitrary ratio within the range of containing organic substances, preferably components derived from the organic structure-directing agent, in the pores. By using a zeolite containing organic substances, preferably components derived from the organic structure-directing agent, in the pores in the present resin composition, a resin composition capable of providing a cured product with low CTE and low hygroscopicity can be provided. When firing is carried out, the firing temperature is preferably usually 200 to 1000 °C. By firing at 300 °C or higher, organic structure-directing agents and the like can be removed. On the other hand, when it is 1000 °C or lower, the physical properties of the zeolite are not impaired. From the above viewpoints, the firing temperature is preferably 300 °C or higher, more preferably 350 °C or higher, still more preferably 400 °C or higher, and preferably 900 °C or lower, more preferably 800 °C or lower, still more preferably 700 °C or lower. The firing atmosphere is not particularly limited, and it may be carried out in air or in an inert gas atmosphere such as nitrogen or argon. The firing method is not particularly limited, and a muffle furnace, a kiln, a fluidized firing furnace, etc. can be used, but a method of firing by circulating the above gas is desirable. The gas flow rate is not particularly limited, but usually the gas flow rate per 1 g of the powder is preferably in the range of 0.1 ml / min or more and 100 ml / min or less, and it is more preferable to carry out firing under a gas flow of 5 ml / min or more and 20 ml / min or less.

[0056] <Resin> The resin in this resin composition is not particularly limited as long as the effects of the present invention are exhibited, and examples include thermosetting resins and thermoplastic resins. Among them, when considering liquid sealants such as underfill materials, it is preferable to contain a thermosetting resin.

[0057] <<Thermosetting resin>> This resin composition preferably contains a thermosetting resin. The thermosetting resin is not particularly limited, and examples include epoxy resins, polyimide resins, maleimide resins, polyamide resins, phenol resins, vinyl ester resins, unsaturated polyester resins, melamine resins, etc. Among these thermosetting resins, in the present invention, it is preferable to contain at least one selected from the group consisting of epoxy resins and polyimide resins, and it is more preferable to contain an epoxy resin.

[0058] (Epoxy resin) As the epoxy resin that can be used in the present invention, since the coefficient of thermal expansion after curing is likely to be low, it is preferable to use an epoxy compound having an aromatic ring such as a bisphenol A type skeleton, a bisphenol F type skeleton, or a biphenyl skeleton. Specifically, bisphenol A type epoxy resin, bisphenol F type epoxy resin, bisphenol S type epoxy resin, biphenyl type epoxy resin, naphthalene ring-containing epoxy resin, epoxy resin having a dicyclopentadiene skeleton, phenol novolak type resin, cresol novolak type epoxy resin, triphenylmethane type epoxy resin, aminophenol type epoxy resin, aliphatic epoxy resin, copolymer epoxy resin of aliphatic epoxy resin and aromatic epoxy resin, etc. are exemplified. Among these, bisphenol A type epoxy resin, bisphenol F type epoxy resin, bisphenol S type epoxy resin, biphenyl type epoxy resin, and naphthalene ring-containing epoxy resin are preferable, and more preferably bisphenol A type epoxy resin, bisphenol F type epoxy resin, naphthalene ring-containing epoxy resin, aminophenol type epoxy resin, and biphenyl type epoxy resin are used.

[0059] Also, as this resin composition, in terms of the glass transition temperature after thermosetting being likely to be high, it is preferable to use a polyfunctional epoxy resin. As the polyfunctional epoxy resin, various phenols such as phenol novolak resin, cresol novolak resin, bisphenol A novolak resin, dicyclopentadiene phenol resin, phenol aralkyl resin, naphthol novolak resin, biphenyl novolak resin, terpene phenol resin, heavy oil-modified phenol resin, etc., and various phenols and various aldehydes such as hydroxybenzaldehyde, crotonaldehyde, glyoxal, etc. Glycidyl ether type polyfunctional epoxy resins such as epoxy resins produced from the obtained polyhydric phenol resins and other various phenolic compounds and epihalohydrin are preferable.

[0060] In addition, from the perspective of fluidity, the viscosity of the epoxy resin at 23°C is preferably 5 Pa·s or less, and more preferably 0.1 to 3 Pa·s. The method for measuring the viscosity of the epoxy resin is specified in JIS K7233 (1986), and the single-cylinder rotational viscometer method is suitable. The viscosity of the epoxy resin used in the present invention at 23°C may be measured using a B-type rotational viscometer (「LVDV-1 Pri」, manufactured by Brookfield, spindle: S62), which is one of the single-cylinder rotational viscometer methods.

[0061] From the perspective of viscosity control, the epoxy equivalent of the epoxy resin is preferably 50 g / eq or more and 500 g / eq or less, and more preferably 90 g / eq or more and 150 g / eq or less. A higher epoxy equivalent is preferable in terms of excellent heat resistance. On the other hand, in terms of the melting point of the epoxy resin being low and the viscosity being low, which results in good fillability of the present resin composition and high bonding properties due to filling, a lower epoxy equivalent is preferable. The epoxy resin may be used alone, or two or more types may be mixed and used in any combination and ratio. However, the epoxy equivalent in the case of mixing shall be the equivalent of the mixture.

[0062] The content of the epoxy resin in the present resin composition is preferably low from the perspective that the content of inorganic fillers such as zeolite becomes relatively high and the coefficient of thermal expansion is easily reduced. On the other hand, a higher content is preferable from the perspective that the excellent physical properties of the epoxy resin are easily maintained. As described above, from the perspective of achieving both the maintenance of the excellent physical properties of the resin and the heat resistance (difficulty of thermal expansion) of the cured resin composition, specifically, it is preferably 5% by mass or more based on the total amount of the resin composition, and more preferably 10% by mass or more. On the other hand, it is preferably 50% by mass or less, more preferably 25% by mass or less, and even more preferably 15% by mass or less.

[0063] (Curing agent) The present resin composition preferably further contains a curing agent. A curing agent refers to a substance that contributes to the cross-linking reaction between the cross-linking groups of a resin, particularly preferably an epoxy resin. There are no particular restrictions on the hardener, and generally those known as resin hardeners, particularly preferably epoxy resin hardeners, can be used. For example, phenolic hardeners, amine-based hardeners such as aliphatic amines, polyetheramines, alicyclic amines, aromatic amines, acid anhydride-based hardeners, amide-based hardeners, tertiary amines, imidazole and its derivatives, organic phosphines, phosphonium salts, tetraphenylboron salts, organic acid dihydrazides, boron halide amine complexes, polymercaptan-based hardeners, isocyanate-based hardeners, blocked isocyanate-based hardeners, dicyandiamide compounds, etc. can be mentioned. From the viewpoints of imparting fluidity and rapid curability, an acid anhydride-based hardener is preferred as the hardener.

[0064] Specific examples of phenolic curing agents include bisphenol A, bisphenol F, 4,4'-dihydroxydiphenylmethane, 4,4'-dihydroxydiphenyl ether, 1,4-bis(4-hydroxyphenoxy)benzene, 1,3-bis(4-hydroxyphenoxy)benzene, 4,4'-dihydroxydiphenyl sulfide, 4,4'-dihydroxydiphenyl ketone, 4,4'-dihydroxydiphenyl sulfone, 4,4'-dihydroxybiphenyl, 2,2'-dihydroxybiphenyl, 10-(2,5-dihydroxyphenyl)-10H-9-oxa-10-phosphaphenanthrene-10-oxide, phenol novolak, bisphenol A novolak, o-cresol novolak, m-cresol novolak, p-cresol novolak, xylenol novolak, poly-p-hydroxystyrene, hydroquinone, resorcinol, catechol, t-butylcatechol, t-butylhydroquinone, fluoroglycinol, pyrogallol, t-butylpyrogallol, allylated pyrogallol, polyallylated pyrogallol, 1,2,4-benzenetriol, 2,3,4-trihydroxybenzophenone, 1,2-dihydroxynaphthalene, 1,3-dihydroxynaphthalene, 1,4-dihydroxynaphthalene, 1,5-dihydroxynaphthalene, 1,6-dihydroxynaphthalene, 1,7-dihydroxynaphthalene, 1,8-dihydroxynaphthalene, 2,3-dihydroxynaphthalene, 2,4-dihydroxynaphthalene, 2,5-dihydroxynaphthalene, 2,6-dihydroxynaphthalene, 2,7-dihydroxynaphthalene, 2,8-dihydroxynaphthalene, allylated or polyallylated products of the above dihydroxynaphthalenes, allylated bisphenol A, allylated bisphenol F, allylated phenol novolak, allylated pyrogallol, etc.

[0065] Specific examples of amine curing agents include, as aliphatic amines, ethylenediamine, 1,3-diaminopropane, 1,4-diaminopropane, hexamethylenediamine, 2,5-dimethylhexamethylenediamine, trimethylhexamethylenediamine, diethylenetriamine, iminobispropylamine, bis(hexamethylene)triamine, triethylenetetramine, tetraethylenepentamine, pentaethylenehexamine, N-hydroxyethylethylenediamine, tetra(hydroxyethyl)ethylenediamine, and the like. Examples of polyetheramines include triethylene glycol diamine, tetraethylene glycol diamine, diethylene glycol bis(propylamine), polyoxypropylene diamine, polyoxypropylene triamines, and the like. Examples of alicyclic amines include isophoronediamine, metaxylylenediamine, N-aminoethylpiperazine, bis(4-amino-3-methyldicyclohexyl)methane, bis(aminomethyl)cyclohexane, 3,9-bis(3-aminopropyl)-2,4,8,10-tetraoxaspiro(5,5)undecane, norbornenediamine, and the like. Examples of aromatic amines include tetrachloro-p-xylenediamine, m-xylenediamine, p-xylenediamine, m-phenylenediamine, o-phenylenediamine, p-phenylenediamine, 2,4-diaminoanisole, 2,4-toluenediamine, 2,4-diaminodiphenylmethane, 4,4'-diaminodiphenylmethane, 4,4'-diamino-1,2-diphenylethane, 2,4-diaminodiphenyl sulfone, 4,4'-diaminodiphenyl sulfone, m-aminophenol, m-aminobenzylamine, benzyldimethylamine, 2-dimethylaminomethylphenol, triethanolamine, methylbenzylamine, α-(m-aminophenyl)ethylamine, α-(p-aminophenyl)ethylamine, diaminodiethyldimethyldiphenylmethane, α,α'-bis(4-aminophenyl)-p-diisopropylbenzene, and the like.

[0066] Specific examples of the acid anhydride-based curing agent include dodecenyl succinic anhydride, polyadipic anhydride, polyazelaic anhydride, polysebacic anhydride, poly(ethyloctadecanedioic) anhydride, poly(phenylhexadecanedioic) anhydride, methyltetrahydrophthalic anhydride, methylhexahydrophthalic anhydride, hexahydrophthalic anhydride, methyl hymic anhydride, tetrahydrophthalic anhydride, trialkyltetrahydrophthalic anhydride, methylcyclohexenedicarboxylic anhydride, methylcyclohexenetetracarboxylic anhydride, phthalic anhydride, trimellitic anhydride, pyromellitic anhydride, benzophenonetetracarboxylic anhydride, ethylene glycol bistrimellitate dianhydride, het acid anhydride, nadic anhydride, methyl nadic anhydride, hydrogenated nadic anhydride, hydrogenated methyl nadic anhydride, 5-(2,5-dioxotetrahydro-3-furanyl)-3-methyl-3-cyclohexane-1,2-dicarboxylic anhydride, 3,4-dimethyl-6-(2-methyl-1-propenyl)-4-cyclohexene-1,2-dicarboxylic anhydride, 3,4-dicarboxy-1,2,3,4-tetrahydro-1-naphthalenesuccinic dianhydride, 1-methyl-dicarboxy-1,2,3,4-tetrahydro-1-naphthalenesuccinic dianhydride, and the like.

[0067] Examples of the amide-based curing agent include dicyandiamide, polyamide resin, and the like. Examples of the tertiary amine include 1,8-diazabicyclo(5,4,0)undecene-7, triethylenediamine, benzyldimethylamine, triethanolamine, dimethylaminoethanol, tris(dimethylaminomethyl)phenol, and the like. Examples of imidazoles and their derivatives include 1-cyanoethyl-2-phenylimidazole, 2-phenylimidazole, 2-ethyl-4(5)-methylimidazole, 2-phenyl-4-methylimidazole, 1-benzyl-2-methylimidazole, 1-benzyl-2-phenylimidazole, 1-cyanoethyl-2-undecylimidazole, 1-cyano-2-phenylimidazole, 1-cyanoethyl-2-undecylimidazole trimellitate, 1-cyanoethyl-2-phenylimidazolium trimellitate, 2,4-diamino-6-[2'-methylimidazolyl-(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 isocyanurate adduct, 2-phenylimidazole isocyanurate adduct, 2-phenyl-4,5-dihydroxymethylimidazole, 2-phenyl-4-methyl-5-hydroxymethylimidazole, and adducts of epoxy resins and the above imidazoles or polymer-encapsulated imidazoles, etc.

[0068] Examples of organic phosphines include tributylphosphine, methyldiphenylphosphine, triphenylphosphine, diphenylphosphine, phenylphosphine, etc. Examples of phosphonium salts include tetraphenylphosphonium tetraphenylborate, tetraphenylphosphonium ethyltriphenylborate, tetrabutylphosphonium tetrabutylborate, etc. Examples of tetraphenylborate salts include 2-ethyl-4-methylimidazole tetraphenylborate, N-methylmorpholine tetraphenylborate, etc. These curing agents may be used alone, or two or more of them may be mixed and used in any combination and ratio.

[0069] When the resin composition contains a curing agent, the content of the curing agent is preferably in the range of 0.8 to 2.0 in terms of the equivalent ratio of the functional group in the curing agent to the epoxy group in the epoxy resin (functional group in the curing agent / epoxy group in the epoxy resin) so that the influence due to the residue of unreacted epoxy groups or functional groups of the curing agent is unlikely to occur. More preferably, it is used in the range of 0.8 to 1.5.

[0070] When the curing agent is an amide-based curing agent, a tertiary amine, imidazole and its derivatives, organic phosphines, phosphonium salts, tetraphenylboron salts, organic acid dihydrazides, boron halide amine complexes, polymer mercaptan-based curing agents, isocyanate-based curing agents, blocked isocyanate-based curing agents, etc., it is preferably used in an amount of 0.1 part by mass or more, more preferably 0.5 part by mass or more, based on 100 parts by mass of the epoxy resin. On the other hand, it is preferably used in an amount of 20 parts by mass or less, more preferably 10 parts by mass or less. In the case of a dicyandiamide compound, it is preferably used in an amount of 0.1 part by mass or more, more preferably 0.5 part by mass or more, based on 100 parts by mass of the epoxy resin. On the other hand, it is preferably used in an amount of 10 parts by mass or less, more preferably 6 parts by mass or less.

[0071] <Reactive diluent> When the resin composition is in a liquid state, the resin composition may contain a reactive diluent. The reactive diluent is not particularly limited as long as it contains at least one monofunctional epoxy compound. The monofunctional epoxy compound is an epoxy compound having one epoxy group and has conventionally been used for adjusting the viscosity of epoxy resin compositions as a reactive diluent. The monofunctional epoxy compound is roughly classified into an aliphatic monofunctional epoxy compound and an aromatic monofunctional epoxy compound, and from the viewpoint of viscosity, it is preferably an aromatic monofunctional epoxy compound.

[0072] <Other additives> In addition to the above, the present resin composition may appropriately contain other additives selected from coupling agents, ultraviolet absorbers, antioxidants, plasticizers, flame retardants, colorants, fluidity improvers, defoamers, ion trap agents, and the like.

[0073] Further, when the present resin composition is in a liquid state, the present resin composition is preferably a solventless system. By using a solventless system, it is possible to prevent the generation of voids and the like due to the volatilization of the solvent when the liquid composition is heat-cured. Here, the solvent is a volatile component, and in this specification, it is a term including water and organic solvents. The solventless liquid composition substantially does not contain a solvent. For example, with respect to the total amount of the liquid composition, the content of the solvent is preferably less than 3% by mass, more preferably less than 1% by mass, and even more preferably 0% by mass.

[0074] <Manufacturing Method of the Present Resin Composition> The present resin composition can be obtained by mixing and kneading zeolite, inorganic fillers other than zeolite, resin, a curing agent, a dispersant, a reactive diluent, and other additive components using a vacuum mixer, a mixing roll, a planetary mixer, etc., and defoaming as necessary. The blending order of these components is arbitrary as long as there are no particular problems such as reactions or precipitates occurring. Among the constituent components, any two components or three or more components may be mixed in advance, and then the remaining components may be mixed, or all the components may be mixed at once.

[0075] <Physical Properties of the Present Resin Composition> (Coefficient of Thermal Expansion (CTE)) When the resin composition is cured to a gel fraction of 80% or more, the average coefficient of thermal expansion (CTE) of the cured product at 25 to 100 °C is preferably 0 ppm / K or more, more preferably 2 ppm / K or more, still more preferably 4 ppm / K or more, and particularly preferably 10 ppm / K or more. On the other hand, it is preferably 100 ppm / K or less, more preferably 50 ppm / K or less, and still more preferably 25 ppm / K or less. Such a resin composition is useful as a material requiring various heat resistances because of its low average coefficient of thermal expansion at temperatures below the glass transition temperature, and is particularly effective for application to electronic devices.

[0076] The above average coefficient of thermal expansion may be measured by thermomechanical analysis for the cured product obtained by curing the resin composition to a gel fraction of 80% or more. Specific measurement conditions are as described in the examples.

[0077] (Viscosity) This resin composition is preferably a composition having fluidity at room temperature (23 °C). The viscosity of this resin composition is preferably low in terms of easy filling even in a narrow space. On the other hand, it is preferably high in terms of difficulty in occurrence of dripping or the like during resin composition filling. The viscosity of this resin composition at 23 °C is preferably 0.1 Pa·s or more, more preferably 1 Pa·s or more, still more preferably 5 Pa·s or more, and particularly preferably 10 Pa·s or more. On the other hand, it is preferably 250 Pa·s or less, more preferably 150 Pa·s or less, and still more preferably 60 Pa·s or less.

[0078] The viscosity at 23 °C may be measured using a B-type rotational viscometer, which is one of the single-cylinder rotational viscometer methods. For example, the B-type rotational viscometer described in the examples may be used.

[0079] (Water absorption rate) It is preferable that the water absorption rate of the cured product when the resin composition is cured to a gel fraction of 80% or more is 15% or less. When the water absorption rate is 15% or less, for example, even when used as a part of an electronic component such as an underfill material, problems caused by hygroscopicity are less likely to occur. From the above viewpoints, the smaller the water absorption rate, the more preferable it is. More preferably, it is 10% or less, still more preferably 5% or less, and particularly preferably 3% or less. The measurement of the water absorption rate can be carried out by the method described in the examples.

[0080] <Use> The present resin composition can be used, for example, in catalyst modules, molecular sieve membrane modules, optical members, moisture-absorbing members, foods, building members, and constituent members and packaging members of electronic devices, etc. Among them, it is preferably used in electronic devices. An electronic device is a device having two or more electrodes and controlling the current flowing between the electrodes or the generated voltage by electricity, light, magnetism, or chemical substances, etc., or a device that generates light, an electric field, or a magnetic field by an applied voltage or current. Specifically, resistors, rectifiers (diodes), switching elements (transistors, thyristors), amplifying elements (transistors), memory elements, or chemical sensors, etc., or devices obtained by combining or integrating these elements can be mentioned. In addition, photodiodes or phototransistors that generate photocurrents, electroluminescent elements that emit light by applying an electric field, and optical elements such as photoelectric conversion elements or solar cells that generate electromotive force by light can also be mentioned. The electronic device is preferably a semiconductor device. The semiconductor device preferably has at least a semiconductor substrate. For example, a device in which a semiconductor chip is mounted on a substrate, a device in which semiconductor chips and semiconductor substrates are laminated in multiple layers, etc. can be mentioned.

[0081] [Liquid encapsulant] When the present resin composition is in a liquid state, it is preferably used as a liquid encapsulant. In that case, the liquid composition is cured to become an encapsulating material. The liquid sealant may be used as a sealing material that fills the gaps formed in the constituent members and then cures to fill the gaps. Note that a method for manufacturing a sealing material having a step of filling the resin composition into the gaps and then curing is also within the scope of the present invention. Further, the liquid sealant may be used, for example, after being applied onto various constituent members, another constituent member is overlaid on the liquid sealant, and then appropriately cured to fill the gaps between the constituent members. At this time, the liquid sealant may be appropriately cured and B-staged before another constituent member is overlaid. Among these, the present resin composition, particularly the liquid composition in which the present resin composition is liquid, is preferably used for the application of filling the gaps and curing. That is, it is preferable to manufacture a sealing material by filling the present resin composition into the gaps and then curing.

[0082] The present resin composition is preferably used as a liquid sealant, and particularly preferably used as an underfill material. The underfill material is preferably used in the manufacture of electric devices, particularly semiconductor devices, and is preferably used for filling the gaps formed, for example, between a substrate and a semiconductor chip, between substrates, and between semiconductor chips. As the substrate, a known substrate can be used, and it is preferable to use a substrate made of an organic material such as an epoxy resin substrate or a phenolic resin substrate. Further, the semiconductor chip is preferably formed from a semiconductor substrate such as a silicon substrate. The cured product of the present resin composition has a low coefficient of thermal expansion. By using it as an underfill material, the difference from the coefficient of thermal expansion of a semiconductor substrate or the like becomes small, so the thermal cycle resistance and the like are improved.

[0083] The underfill material is preferably used, for example, as a sealing material that fills the gap between a substrate and a semiconductor chip in a laminate in which a semiconductor chip is mounted on the substrate and is then cured by heating to seal the space between the substrate and the chip. At this time, the semiconductor chip is preferably joined to the surface of the substrate on which the wiring pattern is formed via bumps, for example, by reflow, before the underfill material is filled.

[0084] The underfill material may be used in the manufacture of semiconductor devices by the pre-apply method. Specifically, on the surface of a semiconductor chip on which a plurality of bumps are formed, an underfill material is filled between the plurality of bumps to form an underfill layer. Here, the filled underfill material may be B-staged as necessary. Thereafter, the semiconductor chip on which the underfill layer is formed may be placed on the surface of the substrate such that the surface on which the underfill layer is formed faces the substrate. Next, by heating, pressurizing, etc., the underfill layer is cured to become a sealing material, and the semiconductor chip is joined to the surface of the substrate on which the wiring pattern is formed via the bumps.

[0085] Also, in the pre-apply method, an underfill material may be applied on the surface of the substrate on which the wiring pattern is formed to form an underfill layer. Here, the applied underfill layer may be B-staged as necessary. Thereafter, the semiconductor chip on which the bumps are formed may be placed on the substrate on which the underfill layer is formed such that the surface on which the bumps are formed faces the surface of the substrate on which the underfill layer is formed. Thereafter, by heating, pressurizing, etc., the underfill layer is cured to become a sealing material, and the semiconductor chip is joined to the surface of the substrate on which the wiring pattern is formed via the bumps.

[0086] In the above description, an example in which the underfill material is used as a sealing material for filling the gap between the substrate and the semiconductor chip has been described. However, the use of the underfill material is not particularly limited, and it may fill the gap between semiconductor chips or may be used as a sealing material for filling the gap between substrates. Also, the substrate is not limited to a substrate made of an organic material and may be a semiconductor substrate or the like.

Examples

[0087] Hereinafter, the present invention will be described in more detail using examples and comparative examples. However, the present invention is not limited to the following examples and comparative examples as long as the gist thereof is not deviated from.

[0088] (Physical property evaluation) The physical property evaluation was carried out as follows.

[0089] (Gel fraction) The gel fraction of the cured product was measured by the following procedure. After heat treatment at 80 °C for 2 hours, the cured product prepared under the curing conditions of 120 °C for 2 hours was cut out within the range of 0.5 to 0.6 g and placed on a wire mesh. The wire mesh was left standing for 24 hours while immersed in acetone. Then, the wire mesh was taken out from the acetone and vacuum dried. The ratio of the weight of the cured product after immersion to the weight before immersion was defined as the gel fraction.

[0090] (Weight loss rate) The weight loss rate of the zeolite was measured by the following procedure. Approximately 5 mg of the zeolite was placed in a platinum cup and introduced into a thermal analyzer (device name; TGA Q5000IR, manufactured by TA Instruments). The temperature was raised from room temperature to 800 °C at a heating rate of 10 °C / min in an air atmosphere and held at 800 °C for 10 minutes. The weight loss rate at 800 °C based on the weight at 400 °C was defined as the weight loss rate. Specifically, it was determined by "weight loss rate of zeolite = 100×{(weight at 400 °C) - (weight when held at 800 °C for 10 minutes)} / (weight at 400 °C)".

[0091] (Average primary particle size) The average primary particle size of the zeolite was measured by the following procedure. The particles were observed with a scanning electron microscope (SEM) (device name; JSM-6701F, manufactured by JEOL). Fifty particles that could be regarded as primary particles were randomly extracted, and for each particle, the diameter of the circle (equivalent circle diameter) with the largest diameter, which had an area equal to the projected area of the particle, was determined. The average value of the equivalent circle diameters of the 50 obtained particles was calculated and defined as the average primary particle size of the zeolite.

[0092] (Circularity of primary particles) The circularity of the primary particles of zeolite was measured by the following procedure. The particles were observed with a scanning electron microscope (SEM) (equipment name: JSM-6701F, manufactured by JEOL Ltd.). For 10 particles that could be regarded as primary particles, the area and circumference were determined, and "circularity = 4×π×area / (circumference) 2 " was calculated. The average value of the circularity values of the 10 obtained particles was calculated and taken as the circularity of the primary particles of zeolite.

[0093] (Sphericity of primary particles) The sphericity of the primary particles of zeolite was measured by the following procedure. The particles were observed with a scanning electron microscope (SEM) (equipment name: JSM-6701F, manufactured by JEOL Ltd.). For 10 particles that could be regarded as primary particles, the maximum diameter and minimum diameter of the particles were determined, and calculated by "the ratio of the minimum diameter to the maximum diameter of the particles". The average value of the sphericity values of the 10 obtained particles was calculated and taken as the sphericity of the primary particles of zeolite.

[0094] (Average coefficient of thermal expansion (CTE) of zeolite) The average coefficient of thermal expansion of zeolite was measured by the following procedure. The pre-dried zeolite was put into an X-ray diffractometer (equipment name: D8 ADVANCE, manufactured by BRUKER) and X-ray diffraction measurement was carried out in the range of 50 to 100°C. The obtained results were used with X-ray diffraction analysis software (software name: JADE, manufactured by Materials Data) to calculate the lattice constants of the a-axis, b-axis, and c-axis at each temperature. The average coefficient of thermal expansion of zeolite was determined by "average coefficient of thermal expansion of zeolite ={(average lattice constant at 100°C)−(average lattice constant at 50°C)} / {(average lattice constant at 50°C)×(100°C−50°C)}". Here, the average lattice constant at each temperature is the average value of the lattice constants of the a-axis, b-axis, and c-axis.

[0095] (Average coefficient of thermal expansion (CTE) of the cured product) The average coefficient of thermal expansion of the cured product when the resin composition was cured to a gel fraction of 80% or more was measured by thermomechanical analysis using a method conforming to JIS K7197 (2012). The measurement was performed by the compression method using a thermomechanical analyzer (apparatus name: TMA SS7100, manufactured by SII NanoTechnology Inc.). Specifically, the cured product when the resin composition was cured to a gel fraction of 80% or more was cut into a size of φ6 mm × 10 mm, and using a thermomechanical analyzer, the temperature was decreased from 200°C to 20°C at 5°C / min by the compression method for measurement. The temperature change of the change in sample length at 25 to 100°C was measured, and the slope of the tangent line was taken as the average coefficient of thermal expansion (CTE).

[0096] (Viscosity) The viscosity of the resin composition at 23°C was measured using a B-type rotational viscometer. As the B-type rotational viscometer, when the viscosity was 0.1 to 100 Pa·s, "LVDV-1 Pri" manufactured by Brookfield Engineering Laboratories, Inc. was used, and spindles S64 and S63 were used. When the viscosity exceeded 100 Pa·s, "HBDV-E" manufactured by Brookfield Engineering Laboratories, Inc. was used, and spindle S-07 was used. The value measured at 5 rpm was taken as the representative value of the viscosity of each sample.

[0097] (Water absorption rate) Regarding the cured product when the resin composition was cured to a gel fraction of 80% or more, after holding in a drying oven at 125°C for 3 hours, it was evaluated by the weight change rate (%) after holding for 3 hours in a constant temperature and humidity chamber adjusted to 85°C and 85% humidity.

[0098] First, examples of the zeolite according to the present invention will be shown.

[0099] Production Example 1 (Production of uncalcined zeolite) To a container, N,N,N-trimethyl-1-adamantylammonium hydroxide (TMAdaOH) manufactured by Seachem as a structure directing agent (SDA), "Kyoward 200S" manufactured by Kyowa Chemical Industry Co., Ltd. as aluminum hydroxide, and "AEROSIL 200" manufactured by Nippon Aerosil Co., Ltd. as silica were sequentially added. The composition and molar ratio of the obtained mixture were SiO 2 :Al 2 O 3 :TMAdaOH:H 2 O = 1.0:0.025:0.4:20. After thorough mixing, the obtained mixture was placed in a pressure-resistant container, and hydrothermal synthesis was carried out in an oven at 150 °C for 48 hours. After suction filtration and washing, it was dried to obtain CHA-type zeolite. The obtained uncalcined zeolite was a zeolite with the particle size of each particle in the range of 1.0 μm or more and 10 μm or less, and its average primary particle size was 3.1 μm. Also, the average thermal expansion coefficient of the uncalcined zeolite at 50 to 100 °C was -5.0 ppm / K, the sphericity was 0.84, and the circularity was 0.840.

[0100] Production Example 2 (Production of Calcined Zeolite) The uncalcined zeolite prepared in Production Example 1 was calcined at 600 °C for 6 hours under air flow to obtain calcined zeolite. The obtained calcined zeolite was a zeolite with the particle size of each particle in the range of 1.0 μm or more and 10 μm or less, and its average primary particle size was 3.1 μm. Also, the average thermal expansion coefficient of the calcined zeolite at 50 to 100 °C was -9.0 ppm / K, the sphericity was 0.85, and the circularity was 0.845. Other physical property values were the same as those of the uncalcined zeolite.

[0101] Next, examples of the resin composition of the present invention will be shown. <Blending Components> The components used for preparing the resin composition are as follows.

[0102] <Epoxy Resin> (A) p-Aminophenol type epoxy resin: manufactured by Mitsubishi Chemical Corporation, product name "jER630", epoxy equivalent: 97 g / equivalent <Hardener> (B) Acid anhydride hardener; acid anhydride (main component: hydrogenated methyl nadic anhydride): manufactured by Shin-Nippon Rika Co., Ltd., product name "Rikacid HNA-100" (acid anhydride equivalent: 174 - 184) <Filler> (C) Zeolite filler; Unfired zeolite and the zeolite produced in Production Example 1 above were used. The weight loss rate measured using a thermal analyzer (apparatus name; TGA Q5000IR, manufactured by TA Instruments, measurement conditions: in air) was 22%. (D) Zeolite filler; Fired zeolite and the zeolite produced in Production Example 2 above were used. The weight loss rate measured using a thermal analyzer (apparatus name; TGA Q5000IR, manufactured by TA Instruments, measurement conditions: in air) was 0.3%. (E) Silica filler; Manufactured by Admatechs Co., Ltd., product name "SC4050-SX" (average particle size 1 μm) <Additive> (F) Additive; Manufactured by BYK-Chemie Japan, wetting dispersant, product name "DISPERBYK-2152" (amino group-containing ultra-high molecular weight polyester, comb type, solvent-free)

[0103] Example 1 The fillers, resin, curing agent, and additive shown in Table 1 were blended in the blending amounts shown in Table 1. Then, using a vacuum mixer (manufactured by EME Co., Ltd., "V-mini 300"), they were mixed at 1500 rpm for 5 minutes to prepare a resin composition (liquid composition). The viscosity of this liquid composition was evaluated by the above method. The results are shown in Table 1. Next, this liquid composition was poured into a mold and heated at 80°C for 2 hours, and then heated at 120°C for 2 hours to cure it to a gel fraction of 80% or more, and then demolded to obtain a cured product. The CTE and water absorption rate of this cured product were evaluated by the above evaluation method. The results are shown in Table 1.

[0104] Example 2 and Comparative Examples 1 to 6 In Example 1, by replacing each component and the blending amount with those shown in Table 1, a resin composition (liquid composition) and a cured product were obtained in the same manner as in Example 1. The results of evaluation in the same manner as in Example 1 are shown in Table 1.

[0105]

Table 1

[0106] From the results of Examples 1 and 2 and Comparative Examples 4 and 5, it was found that by using uncalcined zeolite as the zeolite, compared with the case of using calcined zeolite, the CTE was equivalent, but the viscosity decreased and the water absorption rate decreased. Also, from the comparison with Comparative Example 6 that does not contain silica as an inorganic filler, it was found that the viscosity can be lowered by using uncalcined zeolite and an inorganic filler in combination.

Industrial Applicability

[0107] According to the present invention, it is possible to provide a resin composition having a low coefficient of thermal expansion, low hygroscopicity, and low viscosity after curing. Such a resin composition is suitable as a liquid encapsulant and is particularly useful as an underfill material.

Claims

1. A resin composition comprising zeolite, an inorganic filler other than zeolite, and a resin, The resin composition has a weight loss rate of 1% or more at 800°C based on the weight at 400°C when the zeolite is heated to 800°C at a heating rate of 10°C / min in an air atmosphere and held at 800°C for 10 minutes, as determined by thermogravimetric analysis (TGA).

2. The resin composition of claim 1 , wherein the zeolite has a CBU of d6r.

3. The resin composition according to claim 1 , wherein the zeolite comprises a zeolite having an oxygen ring structure of 8 or less members.

4. The resin composition according to claim 1 , wherein the zeolite comprises a zeolite having a CHA structure.

5. The resin composition according to claim 1 , wherein the sphericity of the zeolite is 0.7 or more.

6. The resin composition according to claim 1, wherein the zeolite has a circularity of 0.800 or more.

7. The resin composition according to claim 1 , wherein the zeolite is an aluminosilicate.

8. The resin composition according to claim 1 , wherein the inorganic filler other than zeolite is silica.

9. The resin composition according to claim 1, wherein the inorganic filler other than zeolite has an average particle size of 0.1 to 5 μm.

10. The resin composition according to claim 1, wherein a mass ratio of the inorganic filler other than the zeolite to the zeolite is 5 / 65 to 40 / 30.

11. The resin composition according to claim 1, wherein the content of the inorganic filler other than the zeolite is 1 to 50 mass %.

12. The resin composition of claim 1 , wherein the resin comprises a thermosetting resin.

13. The resin composition of claim 12 , wherein the thermosetting resin comprises an epoxy resin.

14. A liquid sealant comprising the resin composition according to any one of claims 1 to 13.

15. An underfill material comprising the resin composition according to any one of claims 1 to 13.

16. A method for producing an encapsulant, comprising the steps of filling a gap with the resin composition according to any one of claims 1 to 13 and then curing the composition.

17. An electronic device comprising an encapsulant obtained by the method according to claim 16.

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