Spherical inorganic composition, resin composition, slurry composition, filler for sealing material for semiconductor packaging, and method for analyzing voids of spherical inorganic composition

Abstract

The present invention improves the quality of spherical inorganic composition particles by accurately grasping the properties of voids present in the spherical inorganic composition particles, and provides a spherical inorganic composition suitable as a filler for sealing materials for semiconductor packaging and the like. In the spherical inorganic composition other than a silica monomer, the average particle diameter of the spherical inorganic composition obtained by laser diffraction particle size distribution measurement is 0.1 to 15 μm, and the number of particles of the spherical inorganic composition containing voids having a diameter of 5 μm or more is 50 / mm 3 Hereinafter, the number of particles of the spherical inorganic composition containing voids having a diameter of 10 μm or more is 5 / mm 3 Hereinafter.

Description

Technical Field

[0001] This invention relates to spherical inorganic compositions, resin compositions, slurry compositions, fillers for sealing materials for semiconductor packaging, and methods for analyzing the voids in spherical inorganic compositions, particularly to spherical inorganic compositions having internal voids of types other than silica monomers, and compositions containing such spherical inorganic compositions. Background Technology

[0002] To protect semiconductor IC chips from dust, impurities, and moisture in the air, sealing materials are used to seal the IC chips, thus creating semiconductor packages. Sealing materials primarily use resin compositions composed of resins with high heat and reagent resistance and silicon dioxide with a low coefficient of thermal expansion. Various methods exist for manufacturing semiconductor packages depending on the application and performance requirements. For high-performance, miniaturized packages used in mobile devices, FOWLP (Fan-Out Wafer Level Package) and FOPLP (Fan-Out Panel Level Package) are employed.

[0003] Among the various FOWLP process methods, there is a grinding step to smooth the surface of the semiconductor package containing sealing material after sealing the IC chip. When hollow particles are present in the sealing material, or when voids are created due to air bubbles or other contaminants, depressions form on the ground package surface, leading to reduced yield due to decreased surface smoothness and deteriorated appearance. Particularly in methods where a redistribution layer is formed on the surface of the semiconductor package after grinding, the presence of hollow particles in the sealing material can cause copper wiring to form in the depressions on the package surface. In this state, if the package expands or contracts due to temperature changes, the presence of voids in the depressions can cause the copper wiring to bend and break. Without voids, the copper wiring is surrounded by sealing material, preventing bending even during expansion or contraction. Furthermore, conventionally, copper wiring with linewidths exceeding 10 μm has high rigidity and is not easily bent. However, if the linewidth is reduced to less than 10 μm due to the pursuit of high performance and miniaturization in packaging, the rigidity of the copper wiring decreases. Therefore, reducing the content of hollow particles in sealing materials is receiving attention (see references 1, 2, etc.).

[0004] Regarding packages suitable for servers, their structure and manufacturing methods differ from those described above. The package is mounted in a flip-chip structure on an interposer or similar layer, and then sealed as a whole. Additionally, there are manufacturing methods involving two processes: underfilling with a narrow gap under the chip and overmolding to protect the entire chip. There are also methods that seal both the under-chip and top-chip components as a whole. High fluidity is particularly required to achieve a complete seal. These package types also include a surface polishing process to smooth the surface of the package, and the filler material used for sealing also strongly requires a low content of hollow particles, as described above.

[0005] Existing technical documents

[0006] Patent documents

[0007] Patent Document 1: Japanese Patent Application Publication No. 2022-117398

[0008] Patent Document 2: Japanese Patent Application Publication No. 2021-161008 Summary of the Invention

[0009] To meet the aforementioned requirements, with the miniaturization and micro-wiring of semiconductor packaging, it is necessary to precisely remove solid, coarse particles used in fillers, and the size of these particles is gradually decreasing. Furthermore, the voids within the filler particles need to be minimized; from a quality management perspective, measuring the voids within the filler particles is crucial.

[0010] However, in previous particle porosity measurements, the cross-section of the particles was exposed by grinding them with resin or similar materials. This allowed for the measurement of the solid portion of the particles and the porosity within them. However, the location of the porosity center varies depending on the grinding location and may not be the exact center of the filler, potentially leading to positional deviations. Therefore, even if the filler particles are cut to expose the cross-section, the diameter of the exposed sphere may not be exactly the same, and calculating the porosity size and volume based on the diameter of the cross-section at the off-center position can result in significant errors. Furthermore, errors can also occur due to porosity deformation and blockage caused by the load during grinding. Particularly concerning is the breakage caused by depressions during redistribution layer formation; the larger the volume of the depression, the higher the likelihood of defects. This may be because resin components from the redistribution layer flow into the depressions, causing localized loss of flatness.

[0011] The present invention has been made in view of the above aspects, by accurately grasping the properties of the voids present in spherical inorganic composition particles other than silica monomers, thereby improving the particle quality of spherical inorganic compositions, and thus providing spherical inorganic compositions suitable for resin compositions, slurry compositions, and fillers for sealing materials for semiconductor packaging, and at the same time providing a method for analyzing the voids in spherical inorganic compositions other than silica monomers.

[0012] That is, the spherical inorganic composition of the embodiment, excluding the silica monomer, is characterized in that the average particle size of the spherical inorganic composition, as determined by laser diffraction particle size distribution, is 0.1 to 15 μm, and the number of particles containing voids with a diameter of 5 μm or more in the spherical inorganic composition is 50 per mm. 3 The following refers to 5 particles / mm of spherical inorganic compositions containing voids with a diameter of 10 μm or more. 3 the following.

[0013] Furthermore, in the spherical inorganic composition, the resin composition containing 150 μm was detected by tomographic section analysis when the spherical inorganic composition was filled into the resin material at a solid content concentration of 70% by mass. 3 The above-mentioned porous spherical inorganic composition contains 14 particles per mm. 3 The following is an analysis of fault sections that detected the presence of 35μm. 3 The above-mentioned porous spherical inorganic composition has 50 particles / mm. 3 the following.

[0014] Furthermore, in spherical inorganic compositions, tomographic analysis can be based on X-ray CT or FIB-SEM.

[0015] In addition, the spherical inorganic composition can be composed of alumina, calcium titanate, or silica-alumina composite oxide.

[0016] Furthermore, the uranium content in the spherical inorganic composition can be below 100 ppb.

[0017] In addition, the above-mentioned spherical inorganic composition may contain a silane compound surface treatment.

[0018] Furthermore, the resin composition of the embodiments may have a spherical inorganic composition other than silica monomer and a resin material for dispersing the spherical inorganic composition.

[0019] Furthermore, the slurry composition of the embodiments may have a spherical inorganic composition other than silica monomer and a dispersion medium for dispersing the spherical inorganic composition.

[0020] Furthermore, the filler for the sealing material used in the semiconductor packaging embodiment may contain a spherical inorganic composition other than silicon dioxide monomer.

[0021] The method for analyzing the voids in the spherical inorganic composition according to the embodiments is characterized by comprising: a dispersion step, wherein the spherical inorganic composition, excluding silica monomer, is dispersed in a resin composition; a cross-sectional analysis step, wherein the spherical inorganic composition, together with the resin composition, is subjected to tomographic cross-sectional analysis using X-ray CT or FIB-SEM; and a void calculation step, wherein a three-dimensional image is generated by the tomographic cross-sectional analysis, and the diameter and volume of the voids present in the spherical inorganic composition are calculated.

[0022] Furthermore, in the method for analyzing the voids in the spherical inorganic composition, a curing step for curing the resin composition can be included after the dispersion step.

[0023] The present invention is characterized by a spherical inorganic composition mainly composed of inorganic raw materials other than silica monomers. The average particle size of the spherical inorganic composition, as determined by laser diffraction particle size distribution, is 0.1–15 μm, and the number of particles containing voids with a diameter of 5 μm or more in the spherical inorganic composition is 50 / mm. 3 The following refers to 5 particles / mm of spherical inorganic compositions containing voids with a diameter of 10 μm or more. 3 Therefore, the quality of spherical inorganic particles can be improved by accurately understanding the properties of voids present in spherical inorganic particles other than silica monomers. Furthermore, by applying analytical methods for voids in spherical inorganic compositions, the accuracy of void measurement in spherical inorganic compositions can be improved. Detailed Implementation

[0024] The spherical inorganic compositions, resin compositions, slurry compositions, fillers for semiconductor packaging sealing materials, and methods for analyzing the voids in the spherical inorganic compositions of the embodiments are described below. The spherical inorganic particles (excluding silica monomers) of the embodiments can be dispersed in resin materials to form resin compositions or dispersed in liquid dispersion media to form slurry compositions. They are particularly preferred for use as fillers for semiconductor packaging sealing materials, antenna packaging, etc.

[0025] (Spherical inorganic compositions and fillers for sealing materials in semiconductor packaging)

[0026] The spherical inorganic composition (excluding silicon dioxide monomer) of the embodiment is in particulate form, and these particles can be directly and preferably used as fillers for sealing materials used in semiconductor packaging. As a semiconductor, it is preferably used in products manufactured using FOWLP or FOPLP technologies.

[0027] The spherical inorganic composition of the embodiments is formed from inorganic components other than silica monomer particles, specifically alumina, calcium titanate, or silica-alumina composite oxides, and contains metal oxides such as magnesium oxide, zirconium oxide, and titanium oxide. The required characteristics for the spherical inorganic compositions of alumina, calcium titanate, and silica-alumina composite oxides are as follows.

[0028] Alumina

[0029] In the case of alumina, when grinding the sealing material in a WLP (Wastewater Liquid Layer) to form a redistribution layer, the grinding process exposes the internal voids of the particles filling the sealing material, allowing the resin of the redistribution layer to flow into these voids. This reduces the flatness of the redistribution layer, making it prone to poor conductivity. The amount of particles that increase the internal void volume is crucial in sealing materials for WLP. However, in conventional cross-sectional observations, it is difficult to accurately determine the internal voids of the particles. In contrast, in this embodiment, the voids within the alumina particles can be accurately determined, improving particle precision.

[0030] Calcium titanate

[0031] When calcium titanate is added as a filler to improve its dielectric constant, the inclusion of calcium titanate particles with high porosity can lead to a decrease in dielectric constant. This is particularly true when used in high-frequency communication substrates, where the inclusion of calcium titanate particles with high porosity results in a localized decrease in dielectric constant, leading to increased transmission loss. Therefore, the implementation method allows for accurate control of the porosity of the calcium titanate particles, thereby contributing to improved quality.

[0032] ·Silica-alumina composite oxide

[0033] In the case of silica-alumina composite oxides, such as those used in photosensitive films, lenses, and adhesives for optoelectronic fusion, the strength of the resin material is improved while light transmission is enhanced by matching the refractive index of the filler itself with that of the matrix resin material. When fillers are added in this way, the incorporation of silica-alumina composite oxide particles with high porosity is a major factor leading to fogging. Therefore, in this embodiment, the porosity of the silica-alumina composite oxide can be accurately controlled, mitigating the refractive index issue.

[0034] For the spherical inorganic composition, based on the mass of the composition, it comprises 50% or more of the inorganic composition, preferably 60% or more, 70% or more, 80% or more, 90% or more, or 95% or more. In the spherical inorganic composition of the embodiments, there may be cases where silica monomers are present in the composition due to unavoidable contamination during manufacturing. That is, the use of silica monomers is actively eliminated from the raw materials to remove unavoidable contamination from silica components. However, silica-alumina composite oxides have a crystalline structure composed of silicon, aluminum, and oxygen, and are therefore different from silica monomers (SiO2).

[0035] For calcium titanate, permitted compounds include titanium oxide, iron oxide, molybdenum oxide, and silicon dioxide. Impurities sometimes exist within the calcium titanate crystals, or sometimes as independent particles.

[0036] In spherical inorganic compositions, alumina is known to have α, γ, or θ crystal structures. Calcium titanate is known to have a perovskite structure. The proportion of crystalline components in spherical inorganic compositions varies depending on the species.

[0037] The spherical inorganic composition of silicon dioxide-alumina composite oxide is composed of oxides containing silicon and aluminum (including composite oxides) and has a crystallinity of 0.5% or less. As for the composition ratio of silicon to aluminum, based on the mass of silicon and aluminum, it is preferable that the mass of aluminum is less than 50%, and as an upper limit, more preferably 35%, 30%, 27.5%, 25%, or 20%. Furthermore, based on the molar number of silicon, the molar number of aluminum is preferably 10% or more, more preferably 15% or more, and even more preferably 20% or more.

[0038] For any type of spherical inorganic composition, the size D is determined by laser diffraction particle size distribution. 50 The median particle size is 0.1 μm to 15 μm. As D 50 The lower limit values ​​can be exemplified as 0.2μm, 0.5μm, 1.0μm, and 1.3μm, while the upper limit values ​​can be exemplified as 14.0μm, 11.0μm, 9.0μm, 8.0μm, 7.0μm, and 6.0μm. These upper and lower limit values ​​can be combined arbitrarily.

[0039] D 50 The value is obtained through laser diffraction particle size distribution measurement, representing the particle size reaching 50% of the total volume from the smallest particle size side. Additionally, D... 100 This refers to the particle size reaching 100% on a volume basis, starting from the side with the smaller particle size. It should be noted that D... 50 D 100The value is calculated as a value within the measurement limit of laser diffraction particle size distribution measurement. In reality, there are undetectable coarse and micro particles in laser diffraction particle size distribution measurement. Therefore, there exist particles with a particle size greater than D. 100 The value of the particle size is not contradictory.

[0040] D 50 The value can be controlled by the manufacturing conditions of the spherical inorganic composition. Furthermore, it can be adjusted by a classification process or by adding particle materials with other particle size distributions. The classification process preferably employs centrifugal separation, such as a cyclone separator. The added particle materials are also classified.

[0041] When a spherical inorganic composition is filled into a resin material to achieve a solid content concentration of 80% by mass, the viscosity of the resin composition is below 1500 Pa·s (shear rate of 1 s). －1 The pressure is preferably 1000 Pa·s or less, and more preferably 500 Pa·s or less. As the resin material, an epoxy resin obtained by mixing bisphenol A type epoxy resin and bisphenol F type epoxy resin in a 1:1 ratio is used (for example, ZX-1059 manufactured by Nippon Steel Chemical Materials Co., Ltd.).

[0042] The specific surface area of ​​the spherical inorganic composition is 0.1 m². 2 / g~15m 2 / g. As a lower limit for specific surface area, 0.2m³ can be exemplified. 2 / g, 0.5m 2 / g, 0.8m 2 / g, as the upper limit, can be exemplified by 10m 2 / g, 7m 2 / g, 5m 2 Approximately / g. Specific surface area is a value determined using the BET method with nitrogen. A smaller specific surface area value is preferred as it reduces viscosity when used in slurry compositions, etc. There are no particular limitations on the method for controlling specific surface area. The specific surface area can be adjusted by reducing the amount of micropowder during the synthesis of spherical inorganic compositions and by controlling the residence time in the classifier to a longer duration during classification.

[0043] The voids in the spherical inorganic composition refer to hollow particles, which are bubbles generated during the manufacturing stage of the spherical inorganic composition. Of course, the fewer voids (hollow particles), the better. However, voids are inevitably generated during the manufacturing of the aforementioned spherical inorganic compositions such as alumina, calcium titanate, or silica-alumina composite oxides.

[0044] For voids (hollow particles), based on the condition that the spherical inorganic composition is filled into the resin material at a concentration of 70% by mass of the added solids, the voids have a diameter of 150 μm.3 The above-mentioned porous spherical inorganic composition contains 14 particles per mm. 3 Below, 10 pieces / mm 3 Below, 5 / mm 3 The optimal value is 0 per mm. 3 Below. Simultaneously, it has 35μm 3 The above-mentioned porous spherical inorganic composition has 50 particles / mm. 3 Below, 30 pieces / mm 3 Below, 15 pieces / mm 3 The optimal value is 10 pieces / mm. 3 the following.

[0045] Furthermore, based on the standard that the spherical inorganic composition is filled into the resin material at a solid content concentration of 70% by mass after addition, the number of spherical inorganic composition particles with a pore diameter of 5 μm or more is 50 / mm. 3 Below, 30 pieces / mm 3 Below, 10 pieces / mm 3 The optimal value is 10 pieces / mm. 3 The following is also true. Simultaneously, the number of spherical inorganic particles with pores larger than 10 μm in diameter is 10 per mm. 3 Below, 5 / mm 3 The optimal value is 3 per mm. 3 the following.

[0046] The size of the voids (hollow particles) contained in each particle of the spherical inorganic composition is evaluated by its diameter. To measure the diameter of these voids (hollow particles), the spherical inorganic composition is embedded in resin or the like, the resin block is cut, and the diameter of the voids (hollow particles) is measured based on the cut surface of the spherical inorganic composition exposed at the cross-section. However, when cutting the resin block, since the spherical inorganic composition is dispersed within the resin, the location of the cut surface is entirely random. For example, if the cut surface is located at a position off-center from the sphere, the voids exposed at that cut surface are measured as having a seemingly smaller diameter. It is impossible for all spherical inorganic compositions to be cut precisely at the center of the sphere. Therefore, measuring the size of the voids (hollow particles) based on the cut location lacks rigor.

[0047] Therefore, to accurately measure the size of the voids (hollow particles), it is necessary to know the void diameters of multiple cross-sectional portions of the spherical inorganic composition. In view of this, in this embodiment, tomographic analysis is performed. Specifically, X-ray CT or FIB-SEM is used in the analysis. When using X-ray CT, tomographic sections of the resin block in which the spherical inorganic composition is dispersed (embedded) are photographed. Preferably, the imaging interval (spacing) between sections is a small range, such as less than 1 μm. Based on the photographs of each section, the diameter of the voids (hollow particles) present within each spherical inorganic composition is measured more sensitively. The volume of the voids (hollow particles) is then calculated. It should be noted that even if the shape of the voids is not spherical and is deformed, the volume of the deformed voids can be calculated by integrating the image analysis of the photographs of each section.

[0048] When using FIB-SEM, a resin block containing dispersed (embedded) spherical inorganic compositions is scanned by irradiating with a focused ion beam, and the surface is slowly ground down to a microscale of less than 1 μm. This process sequentially exposes the voids (hollow particles) present within each spherical inorganic composition. The diameter of each void within the spherical inorganic composition is then measured based on the amount of grinding (depth) based on the ion beam irradiation. The volume of the voids (hollow particles) can also be calculated using FIB-SEM, and it can also be used to measure voids with deformed shapes.

[0049] The above measurements were calculated using X-ray CT or FIB-SEM analysis. For X-ray CT or FIB-SEM measurements, measurements were performed at intervals of less than 1 μm to observe the diameter of the largest pore, or three-dimensional data were constructed, and the pore diameter and pore volume within the particle were calculated based on the contrast (brightness) difference between the surrounding resin, spherical inorganic composition, and the pores themselves. Alternatively, X-ray CT data were obtained under conditions where the voxel size was less than 2 μm, and the pore diameter and pore volume within the particle were calculated based on the contrast difference. When using X-ray CT or FIB-SEM analysis, the analysis range was 0.5 mm. 3 above.

[0050] The essential point is to accurately measure the number of hollow particles with large void volumes. In reality, the void volume (capacity) measured using X-ray CT or similar methods, as in the implementation method, deviates from the theoretical spherical volume calculated based on the void diameter. This is because the void shapes within the particles are mostly not true spheres. By performing the tomographic analysis of the implementation method, the diameter and volume of the voids (hollow particles) in each spherical inorganic composition can be accurately detected and calculated. Therefore, the accuracy of quality management of the finished spherical inorganic compositions is improved. This is particularly significant in improving the yield when processing wiring with finer linewidths.

[0051] (Analytical methods for the porosity of spherical inorganic compositions)

[0052] The analytical method for the porosity of the spherical inorganic composition is summarized below. First, the spherical inorganic composition is dispersed (embedded) in a resin composition. The resin uses the composition described above. The concentration of the solids component of the spherical inorganic composition in the resin composition is prepared to be 60–80% by mass, preferably 70% by mass (dispersion step). The purpose of the dispersion step in the resin is to fix the position of each particle of the individual spherical inorganic composition used for subsequent measurement and analysis. Furthermore, after the dispersion step, a curing step is added to solidify the resin composition. This curing step prepares the resin composition as a cured resin by heating the resin composition and irradiating it with ultraviolet light. Of course, the resin composition can be a thermosetting resin or an ultraviolet-curing resin.

[0053] Together with the resin composition, the spherical inorganic composition is subjected to tomographic cross-section analysis using X-ray CT or FIB-SEM (cross-section analysis step). The method of tomographic cross-section analysis is as described above. Three-dimensional images are generated through tomographic cross-section analysis, and the diameter and volume of voids present within the spherical inorganic composition are calculated (void calculation step). The cross-section analysis step and the void calculation step can be performed concurrently, with appropriate adjustments to the analysis range, voxel size, etc., to calculate the maximum diameter and volume of voids (hollow particles) present within each spherical inorganic composition.

[0054] The spherical inorganic composition of the embodiments is preferably surface-treated by a surface treatment agent such as a silane compound or a silazane compound. The silane compound or silazane compound is not particularly limited; a silane compound or silazane compound having appropriate functional groups is selected for surface treatment as needed. Surface treatment is performed by a combination of two or more selected from silane compounds and silazane compounds.

[0055] As a surface treatment, it is preferable to use a surface treatment agent that can incorporate functional groups such as trimethylsilyl, isocyanate, amino, phenyl, phenylamino, vinyl, methacryl, and epoxy groups. For example, titanate coupling agents, aluminate coupling agents, and silane compounds having the functional groups to be incorporated can be reacted.

[0056] Examples of aluminate coupling agents include aluminum acetoalkoxy diisopropyl ester, alkyl aluminum acetoacetate diisopropyl ester, ethyl aluminum acetoacetate diisopropyl ester, tri(ethylacetoacetyl)aluminum, aluminum isopropoxide, aluminum diisopropanol monosec-butoxide, aluminum sec-butoxide, aluminum ethoxide, bis(ethyl acetoacetate) monoacetoacetate aluminum, aluminum triacetylacetone, and aluminum monoisopropoxy monooxyethylacetoacetate.

[0057] As a surface treatment agent, a single compound or a mixture of multiple compounds can be used. The organic functional groups are determined based on the type of resin material and dispersion medium used. There is no particular limitation on the amount used for surface treatment; 0.1 to 5.0 parts by mass are used relative to 100 parts by mass of the spherical inorganic composition.

[0058] For the spherical inorganic composition of the embodiment, the alpha ray generation amount is ideally 0.001 c / cm. 2 •h or less. Particularly ideally, the uranium used as an alpha ray source is 100 ppb or less, more ideally 5 ppb or less, preferably 3 ppb or less, and more preferably 1 ppb or less.

[0059] (Manufacturing method of metal oxide particle materials)

[0060] When manufacturing the spherical inorganic composition of the embodiment, representative manufacturing methods for each component are provided. Furthermore, manufacturing steps, grading steps, and other steps may be used as needed.

[0061] • Manufacturing process (spherical inorganic composition of alumina)

[0062] Various crystalline alumina (alumina) are used as raw material particles, with particles having an average particle size (volume average particle size) larger than that of the final prepared spherical inorganic composition. Furthermore, the desired volume average particle size can be obtained by a pulverizing operation. For example, the particle size distribution is adjusted after pulverizing the coarse raw material particles. Alternatively, the particle size distribution can be adjusted before pulverizing, or even after pulverization. As a control of particle size distribution, it is preferable to remove particles with small particle sizes.

[0063] The coarse raw material particles are preferably manufactured using the VMC method (deflagration process). The VMC method is a method for producing spherical oxide microparticles by utilizing the deflagration phenomenon of metal powder, also known as the "Vaporized Metal Combustion Method." The spherical inorganic compositions of alumina produced by the VMC method exhibit high sphericity, density, and excellent electrical properties. Metallic aluminum is used as the raw material particle. The VMC method involves burning a combustible agent (such as hydrocarbon gas) in an oxygen-containing atmosphere using a burner to create a high-temperature chemical flame. A small amount of raw material particle material, sufficient to form a dust cloud, is then introduced into this chemical flame, causing deflagration to obtain particulate oxides. An atmosphere of 2000°C or higher is preferred as the high-temperature atmosphere.

[0064] The operation of the VMC method is explained as follows: First, a container is filled with a gas containing oxygen as a reactant, forming a chemical flame within this gas. Next, raw material particles are introduced into this chemical flame, forming a dust cloud. The chemical flame then provides heat to the surface of the raw material particles, raising the surface temperature of the metals constituting the particles. Metal vapors contained within the particles diffuse outwards from their surface. These vapors react with oxygen, igniting and producing a flame. The heat generated by this flame further promotes the vaporization of the raw material particles, and the resulting vapors mix with oxygen, leading to a chain reaction of ignition propagation. Therefore, the smaller the particle size of the raw material particles, the larger their specific surface area, and the higher their reactivity, thus reducing the energy required.

[0065] When producing alumina using the VMC process, a mixture of large-particle and small-particle materials is obtained. Therefore, the large-particle component is separated and used as the coarse raw material.

[0066] There are no particular limitations on the pulverization method; common pulverization methods such as jet mills, ball mills, and vibratory ball mills can be used. Jet mills, in particular, are preferred because they introduce fewer impurities from the pulverizing media and have high pulverization efficiency at the micron level. Particle materials produced by the VMC method have high sphericity, and sometimes contain a certain amount of microparticles with a particle size of less than 1 μm in their particle size distribution.

[0067] Particles composed of metal oxides manufactured using the VMC method are used directly or after fractionation as crude raw material particles. Since the metals constituting the raw materials for the VMC method are easier to purify than their metal oxides, it is easier to improve the purity of the raw material particles obtained by the VMC method.

[0068] In addition to preparing spherical inorganic compositions of alumina via the VMC method described above, spherical inorganic compositions of alumina can also be prepared by methods such as flame melting. When preparing spherical inorganic compositions of alumina using the flame melting method, the alumina used as raw material is, for example, pulverized to below 5 μm, and granulated according to the target particle size. Alternatively, heating to above 1000°C can cause the water contained in the crystals to separate and vaporize, thus reducing porosity.

[0069] Utilizing the dust explosion principle of the VMC method, a large quantity of spherical inorganic alumina compositions can be obtained instantaneously. The resulting spherical inorganic alumina compositions form approximately spherical shapes. The particle size distribution of the obtained spherical inorganic alumina compositions can be adjusted by modifying the particle size, quantity, and flame temperature of the raw material particles. Furthermore, the raw material particles can be surface-treated using silane compounds, silazane compounds, etc. There are no particular limitations on the types of silane compounds that can be used; any of the aforementioned surface-treated compounds can be employed.

[0070] The raw material particles are introduced into a flame while dispersed in a carrier, and then combusted. The rate at which the raw material particles are introduced into the flame is not particularly limited. The carrier can be a gas such as nitrogen, argon, or air, or a liquid such as water or alcohol. The method of dispersion is not particularly limited; however, when dispersed in a liquid, it is preferable to introduce the raw material particles into the flame as a mist. For example, it is preferable that the raw material particles contain approximately 10% to 80% of the total volume.

[0071] The flame employs an oxidizing atmosphere. For example, a flame that burns flammable gases such as LPG, ammonia, and hydrogen in an atmosphere with excess oxygen can be cited. Additionally, thermal plasma is also included in the flame. The feed material particles introduced into the flame are vaporized through combustion and then rapidly cooled to form alumina particles. The obtained alumina particles are then recovered using a bag filter or similar method.

[0072] • Manufacturing process (spherical inorganic composition of calcium titanate)

[0073] In the manufacture of the spherical inorganic composition of calcium titanate according to the embodiments, calcium titanate as raw material is prepared into raw material particle material, and particle material with an average particle size (volume average particle size) larger than that of the final prepared spherical inorganic composition is used as coarse raw material particle material. Then, raw material particle material with the desired volume average particle size is produced by a pulverization operation. For example, after pulverizing the coarse raw material particle material, the particle size distribution is adjusted. Alternatively, the particle size distribution can be adjusted before pulverization instead of after pulverization. As for controlling the particle size distribution, it is preferable to remove particles with small particle sizes.

[0074] In manufacturing spherical inorganic compositions of calcium titanate, the raw material particles are heated and melted in a high-temperature atmosphere and then spheroidized, followed by rapid cooling to obtain particles with high sphericity. The high-temperature atmosphere is a temperature above that which softens or melts calcium titanate. The high-temperature atmosphere can be a flame, plasma, or the like, formed by burning a mixture of a combustible gas and an oxidizing gas. Examples of combustible gases include propane, acetylene, and hydrogen. Furthermore, the raw material particles are introduced into the high-temperature atmosphere in a dispersion state dispersed in a carrier. Examples of carriers include inert gases such as nitrogen, oxidizing gases such as oxygen, combustible gases such as propane, water, methanol, isopropanol, and ketones such as acetone.

[0075] It should be noted that surface treatment with silane compounds or silazane compounds can be used when manufacturing spherical inorganic compositions of calcium titanate. Alkyl groups such as phenyl and methyl can be introduced.

[0076] • Manufacturing process (spherical inorganic composition of silica-alumina composite oxide)

[0077] In manufacturing spherical inorganic compositions of silica-alumina composite oxides, the raw material particles are particles containing metallic silicon and metallic aluminum. The metallic silicon and metallic aluminum can be a mixture of distinct particles or an alloy of metallic silicon and metallic aluminum. The purity of the raw material particles directly affects the purity of the spherical inorganic composition; therefore, the purity of the raw material particles is adjusted to the desired level.

[0078] Metallic silicon and metallic aluminum are dissolved in a pharmaceutical solution and then pulverized using an atomizer or similar device to form particulate material. The ratio of metallic silicon to metallic aluminum in the raw material particulate material is approximately the same as that in the manufactured spherical composite oxide particulate material. The average particle size of the raw material particulate material is not particularly limited, and is approximately 0.1 μm to 40 μm.

[0079] Furthermore, the raw material particles are surface-treated. This surface treatment suppresses the aggregation of the raw material particles when they are introduced into a high-temperature oxidizing atmosphere, as described later. Examples of surface treatments include organosilicon compounds such as silane compounds, organoaluminum compounds such as aluminate coupling agents, and organotitanium compounds such as titanate coupling agents.

[0080] In the manufacture of spherical inorganic compositions of silica-alumina composite oxides, the VMC method is used in the same manner as for alumina. As a result, the raw material particles, through a deflagration reaction, transform into oxides. These oxides then settle under gravity and other forces, escaping the high-temperature oxidizing atmosphere and rapidly cooling to form spherical compositions of silica-alumina composite oxides. This composition is then recovered using a bag filter and a cyclone separator.

[0081] Spherical inorganic compositions of silica-alumina composite oxides are surface-treated using surface-treatment agents such as organosilicon compounds (silane compounds), organoaluminum compounds, and organotitanium compounds. In the surface treatment, the surface-treatment agent is brought into direct contact with the surface of the composition (either in liquid or gaseous state), or the surface-treatment agent is brought into contact with the surface of the composition while dissolved in a solvent. Sometimes, heating is performed after surface treatment to promote the reaction between the surface-treatment agent and the surface of the spherical inorganic compositions of silica-alumina composite oxides.

[0082] Grading process

[0083] The grading process involves classifying the spherical inorganic composition prepared from the raw materials until a particle size distribution is achieved, where the content of coarse particles is below the aforementioned upper limit and the content of hollow particles with a diameter of 5 μm or larger is below the aforementioned upper limit. Coarse particles consist of both solid and hollow particles. Grading operations include centrifugation in a gas or solvent, gravity-based separation in solution, and dry or wet sieving methods. Grading is repeated until the target particle size distribution is achieved.

[0084] Centrifugation is a suitable method for removing solid particles from coarse particles. It is desirable to use solvents with low viscosity for centrifugation. Examples include methyl ethyl ketone (MEK), methyl isobutyl ketone (MIBK), and toluene. Solid coarse particles can be separated with high precision by centrifugation at a concentration of approximately 10% to 30% by mass (especially 15% to 25% by mass) dispersed in MEK. Wet centrifugation separates coarse particles by applying centrifugal force to the slurry, causing the coarse particles to settle and be removed.

[0085] To separate coarse particles composed of hollow particles, it is preferable to disperse the lighter hollow particles in a solution before separating them. Separation in solution is preferably performed by allowing the dispersion to stand, applying centrifugal force, and then removing the hollow particles present in the supernatant (hollow particle separation step). The liquid used can be the same type as that used in centrifugal separation. Furthermore, since solid particles in the coarse particle group settle rapidly, while hollow particles settle slowly or not at all, both coarse particles composed of solid and hollow particles can be removed simultaneously by removing the supernatant along with the operation used to remove the aforementioned coarse particles. Additionally, when using a filter for classification, it is performed in the state of a dispersion slurry dispersed in a solvent. It is preferable to perform the classification operation using a filter multiple times. When performing multiple operations, it is preferable to change from a filter with a large pore size to a filter with a small pore size for the classification operation.

[0086] Other processes

[0087] The surface treatments described above belong to other processes. Surface treatments can be selectively combined. Surface treatments can be performed at any time before, after, or during the grading process of the spherical inorganic compositions prepared from the raw materials manufactured through the manufacturing process.

[0088] There is no particular limitation on the amount of surface treatment agent used for surface treatment. For example, when using substances that react with particle surfaces, such as silane compounds or silazane compounds, as surface treatment agents, the amount of reaction with 100%, 75%, 50%, or 25% is selected based on the amount of OH groups present on the surface of the particles to be treated. Alternatively, an excess amount greater than 100% (120%, 150%, etc.) can also be selected. In this case, residual surface treatment agent that does not react with the particle surface remains. As for silane compounds, there are no particular limitations; examples include compounds having phenyl, alkyl, vinyl, methacryloxy, epoxy, phenylamino, amino, or styryl groups.

[0089] (Resin composition)

[0090] The resin composition of the embodiment is a composition obtained by dispersing a spherical inorganic composition prepared from the above-mentioned raw materials (alumina, calcium titanate, silica-alumina composite oxide) in a resin material (including a resin material precursor). The mixing ratio of the spherical inorganic composition to the resin material is not particularly limited. Suitable examples of resin materials include epoxy resin, acrylic resin, and silicone resin. Alternatively, a resin material precursor before curing may also be used.

[0091] (Slurry composition)

[0092] The slurry composition of the embodiment is a composition obtained by mixing a spherical inorganic composition prepared from the above-mentioned raw materials (alumina, calcium titanate, silica-alumina composite oxide) with a liquid dispersion medium (solvent, resin material precursor, etc.). The mixing ratio of the spherical inorganic composition to the dispersion medium is not particularly limited. In addition to the resin material precursors mentioned above, the dispersion medium may also include alcohols such as MEK, MIBK, hexane, and 2-propanol.

[0093] Example

[0094] The spherical inorganic compositions of the embodiments and their manufacturing and analytical methods are prepared and implemented based on the following. Hereinafter, as experimental examples 1 to 15, the preparation process of each experimental example is shown.

[0095] (Experimental Example 1: Alumina)

[0096] Using metallic aluminum with a uranium content below 5 ppb as raw material, spherical alumina was prepared using the aforementioned VMC method. The alumina was then pulverized to an average particle size of 3 μm using a jet mill and spheroidized by rapid cooling in a high-temperature atmosphere (approximately 2000 °C). The resulting spherical alumina was then wet-graded to 5 μm in an aqueous solvent and dried. To achieve the closest packing design, alumina synthesized via the VMC method with an average particle size of 0.2 μm was used in conjunction.

[0097] (Experimental Example 2: Alumina)

[0098] Low-sodium, fragmented alumina with an average particle size of 3 μm was fed into a melting furnace for spheroidization. The resulting spheroidized alumina was then wet-graded in an aqueous solvent to a size of 10 μm and subsequently dried. To achieve the closest packing design, alumina synthesized via the VMC method with an average particle size of 0.2 μm was used in conjunction.

[0099] (Experimental Example 3: Alumina)

[0100] Using metallic aluminum with a uranium content below 5 ppb as raw material, spherical alumina was prepared using the aforementioned VMC method. The alumina was then pulverized to an average particle size of 4 μm using a jet mill and placed in a melting furnace under a high-temperature atmosphere (approximately 2000 °C) for rapid spheroidization. The resulting spherical alumina was then wet-graded in an aqueous solvent to a size of 10 μm before drying. To achieve the closest packing design, alumina synthesized via the VMC method with an average particle size of 0.2 μm was used in conjunction.

[0101] (Experimental Example 4: Alumina)

[0102] Using metallic aluminum with a uranium content of less than 20 ppb as raw material, spherical alumina with an average particle size of 9.8 μm was prepared by the VMC method described above. After wet classification in an aqueous solvent to a particle size of 10 μm, the alumina was dried.

[0103] (Experimental Example 5: Alumina)

[0104] Using metallic aluminum with a uranium content of less than 5 ppb as raw material, spherical alumina with an average particle size of 0.2 μm was prepared by the VMC method described above. After wet classification in an aqueous solvent to achieve a particle size of 5 μm, the alumina was dried.

[0105] (Experimental Example 6: Alumina)

[0106] Using metallic aluminum with a uranium content below 5 ppb as raw material, spherical alumina was prepared using the aforementioned VMC method. The alumina was then pulverized to an average particle size of 1.8 μm using a jet mill and placed in a melting furnace under a high-temperature atmosphere (approximately 2000 °C) for rapid spheroidization. The resulting spherical alumina was then wet-graded in an aqueous solvent to a size of 3 μm and subsequently dried. To achieve the closest packing design, alumina synthesized via the VMC method with an average particle size of 0.2 μm was used in conjunction.

[0107] (Experimental Example 7: Alumina)

[0108] Using metallic aluminum with a uranium content of less than 5 ppb as raw material, spherical alumina with an average particle size of 0.2 μm was prepared by the VMC method described above. After wet classification in an aqueous solvent to a particle size of 3 μm, the alumina was dried.

[0109] (Experimental Example 8: Calcium titanate)

[0110] Calcium titanate particles with an average particle size of 1.5 μm and a fragmented shape were introduced into a melting furnace containing propane gas (a combustible gas) and oxygen (an oxidizing gas) in a flame, along with an air carrier. Due to surface tension during melting, the particles spherically detached from the flame and fell, where they were cooled and solidified. The resulting spherical calcium titanate was recovered and then graded into 5 μm particles using air classifying.

[0111] (Experimental Example 9: Calcium titanate)

[0112] The spherical calcium titanate obtained from the melting furnace in Experimental Example 8 was classified into 5 μm particles using wet fractionation in 2-propanol solvent.

[0113] (Experimental Example 10: Calcium titanate)

[0114] The spherical calcium titanate obtained from the melting furnace in Experimental Example 8 was used directly.

[0115] (Experimental Example 11: Silica-alumina composite oxide)

[0116] Metallic silicon powder with an average particle size of 20 μm and a purity of 99% or higher, and metallic aluminum powder with an average particle size of 25 μm and a purity of 99% or higher, were mixed at a mass ratio of Si:Al = 60:40 (raw material). Following the VMC method described above, propane gas (as a combustible gas) and air (as a combustion-supporting gas) were used in a melting furnace, and the raw material was introduced into a flame under a high-temperature oxidizing atmosphere. Using the VMC method, the metallic material explodes and vaporizes, forming droplets at temperatures below its boiling point and solidifying into spherical particles at temperatures below its melting point. The silica-alumina composite oxide produced during solidification was recovered, and hollow particles were removed by wet gravity separation in an aqueous solvent before drying. Finally, a silica-alumina composite oxide with an average particle size of 0.2 μm was prepared.

[0117] (Experimental Example 12: Silica-alumina composite oxide)

[0118] The spherical silica-alumina composite oxide obtained from the melting furnace in Experimental Example 11 was used directly.

[0119] (Experimental Example 13: Silica-alumina composite oxide)

[0120] Metallic silicon powder with an average particle size of 20 μm and a purity of 99% or higher, and metallic aluminum powder with an average particle size of 25 μm and a purity of 99% or higher, were mixed at a mass ratio of Si:Al = 60:40 (raw material). Following the VMC method described above, propane gas (as a combustible gas) and air (as a combustion-supporting gas) were used in a melting furnace, and the raw material was introduced into a flame under a high-temperature oxidizing atmosphere. Using the VMC method, the metallic material explodes and vaporizes, forming droplets at temperatures below its boiling point and solidifying into spherical particles at temperatures below its melting point. The silica-alumina composite oxide produced during solidification was recovered, and hollow particles were removed by wet gravity separation in an aqueous solvent before drying. Finally, a silica-alumina composite oxide with an average particle size of 0.5 μm was prepared.

[0121] (Experimental Example 14: Silica-alumina composite oxide)

[0122] 40 parts by mass of 2-propanol and 10 parts by mass of tetraethyl orthosilicate were added to 100 parts by mass of aluminum sol 10A manufactured by Kawaken Fine Chemicals Co., Ltd. After reacting at room temperature for 24 hours, the mixture was neutralized with ammonia water to obtain a gel-like precipitate. The precipitate was calcined at 1100°C, slowly cooled, washed with pure water, and dried at 160°C for 2 hours. After drying, the precipitate was pulverized using a jet mill to an average particle size of less than 2 μm. The pulverized material was then further fed into a melting furnace for spheroidization.

[0123] (Experimental Example 15: Silica-alumina composite oxide)

[0124] 40 parts by mass of 2-propanol and 10 parts by mass of tetraethyl orthosilicate were added to 100 parts by mass of aluminum sol 10A manufactured by Kawaken Fine Chemicals Co., Ltd. After reacting at room temperature for 24 hours, the mixture was neutralized with ammonia water to obtain a gel-like precipitate. The precipitate was washed with pure water and dried at 160°C for 2 hours. After drying, it was pulverized using a jet mill to an average particle size of less than 2 μm. The pulverized material was then fed into a melting furnace for spheroidization.

[0125] (Experiment 16: Glass)

[0126] Glass powder with an average particle size of 21 μm was crushed to an average particle size of 2.3 μm and then fed into a melting furnace for spheroidization.

[0127] (Particle size distribution determination)

[0128] For each test example, the particle size after pulverization and melting was measured in an aqueous solution using a Shimadzu SALD-7500 nano laser diffraction particle size distribution measuring device manufactured by Shimadzu Corporation. D was then calculated. 10 D 50 (Median particle size), D 90 Particle size distribution.

[0129] (Specific surface area determination / BET method)

[0130] Weigh 1.0 g of each test sample and add it to the sample cell for measurement. After pretreatment, the BET specific surface area value is determined using the nitrogen adsorption method. The determination is performed using the Shimadzu TriStar (registered trademark)-II 3020 automatic specific surface area and pore size distribution measuring device manufactured by Shimadzu Corporation. The pretreatment conditions are as follows.

[0131] Degassing temperature: 300℃

[0132] Degassing time: 30 minutes

[0133] Cooldown time: 4 minutes

[0134] (Component Analysis)

[0135] When analyzing the atomic composition of each test sample, an ICP-MS (inductively coupled plasma atomic emission spectrometry) device manufactured by Shimadzu Corporation was used for the determination of U. During the determination, each test sample was prepared by completely dissolving it in a mixture of nitric acid and hydrofluoric acid, and then supplied to the apparatus.

[0136] (Content of hollow particles larger than 5μm obtained through cross-sectional observation)

[0137] Liquid epoxy resin ZX1059 (manufactured by Nippon Steel Chemical Materials Co., Ltd.) and the spherical inorganic composition (filler) prepared in the test example were mixed, and then curing agent ETHACURE 100 (manufactured by Mitsui Fine Chemicals Co., Ltd.) was added and mixed. At this time, the spherical inorganic composition (filler) was prepared to 70% by mass. The mixture of resin and spherical inorganic composition was heated to 170°C to cure the resin. After curing, the cured resin was cut and the cross-section was ground.

[0138] Ion beam milling was performed using an ArBlade 5000 (Hitachi High Technology Co., Ltd.), and the cross-section was osmium-coated with osmium tetroxide gas before observation using SEM. The measurement and observation range was 9 mm. 2 The number of pore-filled particles contained in a spherical inorganic composition with a diameter (major axis) of 5 μm or more.

[0139] (Content of hollow particles larger than 5μm obtained by X-ray CT observation)

[0140] Liquid epoxy resin ZX1059 (manufactured by Nippon Steel Chemical Materials Co., Ltd.) was mixed with the spherical inorganic composition (filler) prepared in the test example, and then curing agent ETHACURE 100 (manufactured by Mitsui Fine Chemicals Co., Ltd.) was added and mixed. At this time, the spherical inorganic composition (filler) was prepared to 70% by mass. The mixture of resin and spherical inorganic composition was heated to 170°C to cure the resin. After curing, the cured resin was cut and the cross-section was ground.

[0141] The cured resin was scanned using a microfocus X-ray CT scanner (Rigiku Co., Ltd., nano-3DX). The settings were 0.64 μm / voxel and the measurement range was 0.58 mm. 3 The scanned images were processed using the analysis software VG Studio MAX to calculate the pore volume inside the spherical inorganic composition. Then, for a 35 μm... 3 150μm 3 The above number of gaps is counted.

[0142] (Content of coarse particles)

[0143] The spherical inorganic compositions prepared in each test example were sieved using a sieve with a mesh size of 10 μm or 5 μm. Then, the mass before sieving and the mass of particles remaining on the sieve were measured. Test examples with a residue amount of less than 500 ppm were evaluated as "0", and test examples with a residue amount of more than 500 ppm were evaluated as "×".

[0144] (Filling)

[0145] Liquid epoxy resin ZX1059 (manufactured by Nippon Steel Chemical Materials Co., Ltd.) was mixed with the spherical inorganic composition (filler) prepared in the test example. At this point, the spherical inorganic composition (filler) was prepared to a concentration of 80% by weight (mass %). The rheometer ARES-G2 (manufactured by TA Instruments) was used to measure the rheological properties (shear rate 1 s). －1 ) Viscosity at 25°C. Then, evaluate whether it is below 1500 Pa·s. 1500 Pa·s or below is rated as "0", and 1500 Pa·s or above is rated as "×".

[0146] (result)

[0147] The results are shown in Tables 1, 2, 3, and 4 below. From top to bottom, the results are: species, average particle size (μm), specific surface area (m²), etc. 2 / g), the number of hollow cells larger than 5μm observed in cross-section (cells / cm²) 2 Hollow content of 10μm and above (cells / cm) 2 ), pore volume 35μm 3 The above particles (number / cm) 2 ), pore volume 150μm 3 The above particles (number / cm) 2 "The number of hollow cells larger than 5μm (cells / mm) observed by X-ray CT" 3 Hollow content of 10μm and above (cells / mm) 3 ), pore volume 35μm 3 The above particles (number / mm) 3 ), pore volume 150μm 3 The above particles (number / mm) 3 ) , filling (0 or ×) and U (uranium) content (ppb) items.

[0148]

[0149]

[0150]

[0151]

[0152] (Inspection)

[0153] For spherical inorganic compositions, the smaller the average particle size (the finer the particle size), the lower the proportion of hollow particles with large internal void volumes. However, fine particles reduce the filling properties of the resin. Therefore, they are unsuitable for filler applications. Furthermore, in applications using semiconductor sealing materials (fillers for semiconductor packaging sealing materials), filling properties are crucial for controlling the coefficient of thermal expansion. To balance both aspects, spherical inorganic compositions can achieve sufficient filling properties by having an average particle size of 0.5 μm or more.

[0154] In wafer-level packaging (WLP), when a redistribution layer is formed on a ground sealing material, the grinding process exposes the internal voids of the particles filling the sealing material. Resin from the redistribution layer can flow into these voids, reducing the flatness of the redistribution layer and increasing the likelihood of poor conductivity. Therefore, understanding the content of particles with large internal void volumes is crucial for sealing materials used in wafer-level packaging (WLP). Conventional cross-sectional observation methods struggle to accurately determine the internal voids of particles. In contrast, as disclosed in the examples, tomographic analysis can measure the internal voids of spherical inorganic compositions, improving the accuracy of evaluation. This is particularly effective in addressing the aforementioned wafer-level packaging problems in the case of spherical inorganic compositions containing alumina.

[0155] Spherical inorganic compositions of calcium titanate are advantageous for applications involving the improvement of dielectric constant. When fillers are added to increase the dielectric constant, the incorporation of particles with high hollowness can lead to a decrease in dielectric constant. This is particularly problematic when used as fillers in high-frequency communication substrates, where the incorporation of particles with high hollowness can cause localized decreases in dielectric constant, resulting in increased transmission loss. Therefore, the spherical inorganic compositions of calcium titanate described in this embodiment reduce the hollowness, thus addressing the issue of dielectric constant modulation.

[0156] Spherical inorganic compositions of silica-alumina composite oxides are examples of fillers suitable for use as materials in optical systems. For instance, in photosensitive films, lenses, and adhesives used in photoelectric fusion, the refractive index of the filler itself is matched to the matrix resin material. When fillers are added to improve the strength of the resin material while transmitting light, the incorporation of particles with high hollowness is a major factor leading to fogging, reducing light transmittance and sensitivity. In response, the spherical inorganic compositions of silica-alumina composite oxides of the embodiments reduce the hollowness, decrease diffuse reflection, and thus address the fogging problem.

Claims

1. A spherical inorganic composition, characterized in that, The main components are inorganic raw materials other than silicon dioxide monomers. The average particle size of the spherical inorganic composition, as determined by laser diffraction particle size distribution analysis, is 0.1–15 μm. The spherical inorganic composition containing pores with a diameter of 5 μm or more has 50 particles / mm. 3 the following, The spherical inorganic composition containing pores with a diameter of 10 μm or more has a particle size of 5 particles / mm. 3 the following.

2. The spherical inorganic composition according to claim 1, characterized in that, The resin composition in which the spherical inorganic composition is filled into the resin material at a solid content concentration of 70% by mass was analyzed by tomographic section analysis, and the detected content was 150 μm. 3 The above-mentioned spherical inorganic composition has 14 particles / mm in its pores. 3 the following, The 35μm content detected by the fault section analysis 3 The number of particles in the above-mentioned spherical inorganic composition with voids is 50 per mm. 3 the following.

3. The spherical inorganic composition according to claim 2, wherein, The fault section analysis is based on X-ray CT or FIB-SEM.

4. The spherical inorganic composition according to claim 1, wherein, The spherical inorganic composition is composed of alumina, calcium titanate, or a silica-alumina composite oxide.

5. The spherical inorganic composition according to claim 1, wherein, The uranium content in the spherical inorganic composition is less than 100 ppb.

6. The spherical inorganic composition according to claim 4, wherein, The spherical inorganic composition comprises a surface treatment of a silane compound.

7. A resin composition, characterized in that, The spherical inorganic composition of claim 1 and the resin material for dispersing the spherical inorganic composition.

8. A slurry composition comprising the spherical inorganic composition of claim 1 and a dispersion medium for dispersing the spherical inorganic composition.

9. A filler for a sealing material used in semiconductor packaging, characterized in that, Contains the spherical inorganic composition according to claim 1.

10. A method for analyzing the porosity of a spherical inorganic composition, characterized in that, It has the following processes: The dispersion process involves dispersing spherical inorganic components, excluding silica monomers, into the resin composition. The cross-sectional analysis process involves performing tomographic cross-sectional analysis of the spherical inorganic composition, together with the resin composition, using X-ray CT or FIB-SEM. The void calculation process involves creating a three-dimensional image through the analysis of the fault section to calculate the diameter and volume of the voids present in the spherical inorganic composition.

11. The method for analyzing the porosity of the spherical inorganic composition according to claim 10, wherein, Following the dispersion step, there is a curing step that cures the resin composition.

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