Filling material for semiconductor mounting material, method for producing the same, and semiconductor mounting material

Abstract

The present invention provides a method for producing a filler for electronic materials with excellent performance. A combustion process is provided in which a raw particle material is introduced into a flame obtained by combusting a non-carbon-containing combustible non-carbon-containing gas to form a particle material contained in the filler for electronic materials. By using a non-carbon-containing combustible gas as the combustible gas, the generation of conductive particles formed from carbon is eliminated in principle. Therefore, a process for removing conductive particles composed of carbon by sieving or the like is not required. In particular, carbon from a hydrocarbon gas sometimes adheres to the surface or the like of the particle material or is formed in the interior of the particle material, and thus, sieving or the like cannot completely remove it, but the production method of the present invention can prevent the mixing of carbon in principle.

Description

Technical Field

[0001] This invention relates to fillers for semiconductor mounting materials, methods for manufacturing the same, and semiconductor mounting materials. Background Technology

[0002] In conventional semiconductor mounting materials, such as printed wiring substrates, electronic substrates, solder resists, interlayer insulating films, construction materials, FPC adhesives, chip soldering materials, underfill materials, ACF, ACP, NCF, NCP, and sealing materials, resin compositions consisting of inorganic particle materials dispersed in resin materials are commonly used. Since semiconductor mounting materials are in direct contact with semiconductors, they require various properties such as high electrical properties (e.g., high insulation resistance) and low mechanical properties (e.g., low coefficient of linear expansion). These high performance characteristics are achieved by dispersing inorganic particle materials in resin materials (e.g., Patent Document 1).

[0003] As the particle material, it is preferable to use a particle material composed of metal oxides (oxide particle material), especially by using a particle material with high sphericity, which can improve the filling performance of the particle material, and is therefore preferred.

[0004] Methods for manufacturing particle materials with high sphericity include: the so-called VMC method, which involves immersing a metal particle material (metal particle material) in a flame and burning it to produce a particle material composed of metal oxides; and the melting method, which involves immersing a raw material particle material composed of metal oxides in a flame and melting it, and then cooling the resulting material to produce a particle material.

[0005] In the VMC process, metal particles undergo explosive combustion in a flame, resulting in the vaporization of metal oxides, which are then cooled to produce oxide particles with extremely high sphericity. The flame used in this process is formed by mixing combustible gases such as propane with combustion-supporting gases such as oxygen and then allowing them to burn.

[0006] In addition, the metal particles that constitute the raw materials for the VMC process have the following characteristics: they are relatively easy to purify, and it is also easy to obtain high-purity materials for the resulting oxide particles.

[0007] In contrast, in the melting method, the metal oxide particles used as raw materials are spheroidized by melting and cooling. Therefore, there are fewer restrictions on the raw materials, and particle materials can be manufactured from a wide variety of raw materials.

[0008] Existing technical documents

[0009] Patent documents

[0010] Patent Document 1: Japanese Patent Application Publication No. 2020-111474 Summary of the Invention

[0011] However, with the miniaturization of semiconductors in recent years, high-performance particulate materials dispersed in semiconductor mounting materials are required. For example, in applications involving direct semiconductor contact where wiring miniaturization has made progress, if conductive particles (conductive particles) are mixed in as impurities, short circuits may occur between adjacent wirings. Therefore, it is necessary to reduce the amount of conductive particles. Thus, the inventors have aimed for further high purity of oxide particulate materials manufactured using the VMC method and melt method.

[0012] The present invention was made in view of the above-mentioned actual situation, and the problem to be solved is to provide a filler for semiconductor mounting materials with superior performance than before, a method for manufacturing the same, and a semiconductor mounting material.

[0013] To address the aforementioned issues, the inventors conducted in-depth research, focusing on the composition of the combustible gas used in the VMC and melting processes. Conventionally, hydrocarbon gases such as propane were used as the combustible gas in the VMC and melting processes. These hydrocarbon gases are burned into carbon dioxide and water, and partially become carbon through incomplete combustion, which is then incorporated into the manufactured particulate material. Therefore, it is understood that by using combustible gases that do not contain carbon (non-carbon-containing gases), such as hydrogen or ammonia, instead of hydrocarbon gases as the combustible gas, conductive particles such as carbon will not be generated even if incomplete combustion occurs.

[0014] Furthermore, it is evident that, particularly when ammonia is used as a non-carbon-containing gas, it is possible to manufacture particulate materials with preferred properties derived from ammonia.

[0015] Based on the above insights, the inventors have made the following invention. That is, the method for manufacturing a semiconductor mounting material filler of the present invention, which solves the above-mentioned problems, is a method for manufacturing a semiconductor mounting material filler comprising particulate materials dispersed in a resin material to form a semiconductor mounting material.

[0016] The particle material is mainly composed of the following metal oxides: the supernatant containing carbon-containing foreign matter larger than 20 μm in the size of a dispersion prepared by dispersing 50 g in 400 mL of ethanol is irradiated with ultrasound at 38 kHz and 300 W for 20 minutes and allowed to stand for 24 hours contains less than 10 particles, the volume average particle size is 0.1 μm to 40 μm, and the sphericity is greater than 0.85.

[0017] The manufacturing method includes the following spheroidizing step: a raw material particle material, whose main components are the metal contained in the above-mentioned metal oxide and / or the metal oxide, is fed into a flame for combustion and / or melting to form the above-mentioned particle material. The flame is obtained by burning a combustible gas, which contains more than 20% by volume a non-carbon-containing combustible gas that does not contain carbon.

[0018] By including more than 20% non-carbon-containing gas by volume in the combustible gas, the generation of conductive particles composed of carbon is reduced in principle. In particular, by making the combustible gas entirely non-carbon-containing, the generation of conductive particles is virtually eliminated. Therefore, the process of removing conductive particles composed of carbon by means of sieving or the like is eliminated, and the removal of conductive particles becomes easy. In particular, carbon from hydrocarbon gases sometimes adheres to and forms on the surface of the manufactured particle material or forms inside the particle material. Therefore, there are cases where sieving or the like cannot completely remove it. However, using the manufacturing method of the present invention, the contamination of carbon can be prevented or even suppressed in principle.

[0019] Furthermore, in the method for manufacturing the particle material of the present invention, in particular if ammonia is used as a non-carbon-containing gas, the following side effects will also occur.

[0020] The first side effect is the ability to include small-sized particles. Including small-sized particles improves flowability. Compared to hydrocarbon gases, ammonia produces less heat through combustion; therefore, a larger volume is required to generate the same amount of heat. As a result, the flame size can be increased, allowing for reliable combustion of the raw material particles and improving the sphericity of the produced particles. Furthermore, the low temperature of the flame formed using ammonia slows down particle growth within the flame, enabling the inclusion of small-sized particles.

[0021] The second side effect is that when using silicon dioxide as a particle material, Si-N bonds can be introduced into the particle material. Although the Si-N bond has the same bond energy as the Si-O bond, which is the main bond in silicon dioxide, O has two bonding sites, while N has three. This increases the relative bond energy per unit mass (or unit volume) of the particle material, and can be expected to increase the hardness, refractive index, and acid and alkali resistance of the particle material.

[0022] The third side effect is that the amount of water generated per unit of heat from the combustible gas increases relatively, thereby increasing the amount of hydroxyl groups on the surface of the metal oxide particle material. This can lead to an increase in reaction sites for surface treatment using coupling agents, etc., and improved adhesion to the resin.

[0023] The particle material of the present invention, which solves the above-mentioned problems, is mainly composed of the following metal oxide: after irradiating the dispersion of 50g in 400mL of ethanol with ultrasound at 38kHz and 300W for 20 minutes and allowing it to stand for 24 hours to allow the particle material to settle naturally, the supernatant contains no more than 10 carbon-containing colored foreign matter larger than 20μm, has a volume average particle size of 0.1μm to 40μm, and a sphericity of 0.85 or higher.

[0024] Colored foreign matter refers to substances whose color differs from that of ordinary metal oxide particles. Whether a substance is colored is determined by its appearance under a microscope. Specifically, this is determined by comparing the supernatant with the particles contained in the separated precipitate to see if they are colored. It should be noted that the particle size of the colored foreign matter is preferably less than twice the volume average particle size of the particles. The presence or absence of carbon can be determined by energy-dispersive X-ray analysis (EDX). When the carbon content detected by EDX is 1 atom% or more, it is considered to contain carbon. In particular, the carbon in question in this specification is conductive carbon such as that found in coal or graphite. When the question is about the presence or absence of carbon, it is preferable to detect and treat the presence or absence of coal or graphite-like carbon as the issue.

[0025] In the VMC method and melt method, which are common methods for manufacturing particulate materials composed of metal oxides, particulate materials are manufactured by throwing raw material particulate materials composed of metals or metal oxides into a flame. As the combustible gas that forms the flame, hydrocarbon gases such as propane are used. Therefore, the contamination of colored foreign matter containing carbon from hydrocarbon gases is unavoidable. Detailed Implementation

[0026] The following describes in detail the semiconductor mounting material filler and its manufacturing method, as well as the semiconductor mounting material itself, based on embodiments. The semiconductor mounting material filler of this embodiment is used by dispersing it in a resin material. Examples of semiconductor mounting materials include printed wiring substrate materials, electronic substrates, solder resists, interlayer insulating films, construction materials, FPC adhesives, chip soldering materials, underfill materials, ACF, ACP, NCF, NCP, and sealing materials. It should be noted that in this specification, "particle size" refers to the volume average particle size relative to the aggregate of particle materials; when referring to individual particle materials, it refers to the individual particle size of each particle material.

[0027] (Semiconductor mounting material filler and semiconductor mounting material)

[0028] The semiconductor mounting material of this embodiment is formed by dispersing a filler in a resin material. The filler for the semiconductor mounting material of this embodiment may consist partly or entirely of the particulate material described later. The resin material is not particularly limited and examples include epoxy resin and silicone resin. A thermosetting resin prior to curing is particularly preferred. Based on the overall mass, the filler for the semiconductor mounting material preferably contains approximately 20% to 92% of the resin material, more preferably approximately 40% to 90%, and even more preferably approximately 60% to 88%.

[0029] The particle material constituting the semiconductor mounting material filler of this embodiment (hereinafter referred to as "the particle material of this embodiment") is mainly composed of metal oxides. Examples of metal oxides include silicon dioxide, aluminum oxide, titanium dioxide, zirconium oxide, mixtures thereof, and composite oxides thereof. In particular, based on the overall mass, it is preferable to contain 50% or more, 60% or more, 70% or more, 80% or more, 90% or more, 95% or more, or 99% or more of silicon dioxide, and more preferably, it is composed entirely of silicon dioxide except for unavoidable impurities.

[0030] When silicon dioxide is used as the metal oxide, the particle material preferably has Si-N bonds. The presence of Si-N bonds is determined by the presence of nitrogen. There is no particular limitation on the nitrogen content; as long as the nitrogen content is 0.1 at% or more based on the total mass of the particle material, it is considered that Si-N bonds are present.

[0031] The volume average particle size of the particle material in this embodiment is 0.1 μm to 40 μm. The volume average particle size is determined by laser diffraction. The upper limit of the volume average particle size is preferably 40 μm, 20 μm, 10 μm, or 5 μm, and the lower limit is preferably 0.1 μm, 0.3 μm, 0.5 μm, or 2 μm. These upper and lower limits can be combined arbitrarily.

[0032] The sphericity of the particle material in this embodiment is preferably 0.85 or higher, 0.88 or higher, 0.90 or higher, 0.95 or higher, or 0.97 or higher. The sphericity is measured using an image analysis device FPIA-3000 (manufactured by Sysmex Corporation).

[0033] Particle materials can undergo surface treatment. Surface treatment allows for the optimization of the surface properties of the particle materials. For example, when mixed with a resin material, hydrophobication (phenyl, hydrocarbon groups, etc.) can be performed to improve affinity with the resin, or functional groups that react with the resin (vinyl, epoxy, acrylic, methacrylic, etc.) can be introduced. The amount of surface treatment is not particularly limited; surface treatment can be performed in a manner that achieves the desired properties. Furthermore, when the surface treatment agent is a substance that reacts with functional groups (OH groups, etc.) on the surface of the filler material, the amount of the surface treatment agent (total amount, half amount, multiple amount, etc. of functional groups on the surface) can be selected based on the amount of functional groups present on the surface of the filler material.

[0034] Surface treatment agents for surface treatment can be silane compounds. Examples of silane compounds include substances called silane coupling agents that have SiH, SiOH, or SiOR (R being a hydrocarbon group), or silazanes such as hexamethylenedisilazane. Examples also include compounds in which any functional group is bonded to the Si group of the silane compound.

[0035] Examples of any functional group include hydrocarbon groups (alkyl groups (methyl, ethyl, propyl, butyl, etc.), alkenyl groups (vinyl, ethenyl, propenyl, etc.), phenyl, amino, phenylamino, acrylate, methacrylate, epoxy, styrene, organosilicon, and combinations thereof. As a silane compound, one type or a combination of two or more can be used for surface treatment. When combining two or more types for surface treatment, multiple surface treatment agents can be mixed for surface treatment, or multiple surface treatment agents can be used sequentially for surface treatment.

[0036] The particle material in this embodiment preferably has a crystallinity of 3% or less. Crystallinity is calculated from the area of ​​the peaks from the crystalline material and the area of ​​the peaks from the amorphous material, based on the spectrum measured by XRD. The peaks from the crystalline material are derived from a Powder Diffraction File provided by the International Data Center for Diffraction.

[0037] In this embodiment, the number of colored foreign matter larger than 20 μm in the particle material, as determined by the following method, is 10 or less per 50g, preferably 8 or less per 50g, 6 or less per 50g, 4 or less per 50g, or 2 or less per 50g. It should be noted that the upper limit for the number of colored foreign matter may be further increased, but based on the results of comparative examples, it can be inferred that even upper limits such as 30 or less per 50g, 25 or less per 50g, 20 or less per 50g, or 15 or less per 50g can sometimes achieve sufficient performance.

[0038] The quantity of colored foreign matter was determined as follows: A dispersion of 50g of particulate material dispersed in 400mL of ethanol (as the dispersion medium) was irradiated with ultrasound at 38kHz and 300W for 20 minutes. The supernatant, after standing for 24 hours, was filtered through a 20μm nylon mesh sieve, and the quantity of foreign matter remaining on the mesh was measured. Whether the colored foreign matter contains carbon was determined using the method described above.

[0039] (Methods for manufacturing particle materials)

[0040] The particle material manufactured by the particle material manufacturing method of this embodiment is the particle material of this embodiment described above. Therefore, a description of the manufactured particle material is omitted. The particle material manufacturing method of this embodiment includes a spheroidizing step of immersing the raw material particle material in a flame to burn and / or melt it. The raw material particle material is composed of a metal and / or the metal oxide corresponding to the type of metal oxide constituting the manufactured particle material. For example, in the case where the metal oxide is silicon dioxide, the raw material particle material contains metallic silicon, or contains silicon dioxide, or contains both metallic silicon and silicon dioxide. The manufacturing method of this embodiment can be carried out in a furnace formed of an appropriate size and material. It is preferable that no carbon-based particles remain in the furnace.

[0041] Combustible gases used as fuel are gases that can form flames at temperatures higher than those that can react with oxygen or other combustion-supporting gases to melt metal oxides, and that can react with metals that are the raw materials for metal oxides.

[0042] The combustible gas comprises, in part or in whole, non-carbon-containing gases such as hydrogen and ammonia. Based on the total volume of the combustible gas, it contains more than 20% non-carbon-containing gas, preferably more than 40%, more preferably more than 60%, further preferably more than 80%, and particularly preferably 100% non-carbon-containing gas.

[0043] Here, when using hydrogen and ammonia as non-carbon-containing gases, they can be used individually or as a mixture. That is, the hydrogen:ammonia ratio in the non-carbon-containing gas can be arbitrarily set within the range of 10:0 to 0:10, for example, in ratios of 9:1, 8:2, 7:3, 6:4, 5:5, 4:6, 3:7, 2:8, 1:9, etc. Alternatively, it can contain non-carbon-containing gases other than hydrogen and ammonia.

[0044] The raw material particles can be obtained by atomizing metals or metal oxides using an atomizer, pulverizer, granulator, or similar equipment. For example, the raw material can be heated and melted, then atomized using an atomizer. The raw material particles can then be obtained by pulverizing materials larger than the raw material particles. Alternatively, materials smaller than the raw material particle size can be granulated to achieve the desired size. It should be noted that when granulation is performed, a carbon-free binder is preferably used. For example, granulation can be performed without a binder by spray drying a dispersion in water.

[0045] For purposes such as improving the flowability of the raw material particles, the raw material particles may also undergo the surface treatments described in the particle material section. The particle size of the raw material particles is not particularly limited, and a particle size distribution similar to that of the manufactured particle material can be adopted. Furthermore, D90 / D10 is preferably 3 or less, and more preferably 2 or less. It should be noted that D10 and D90 are the particle sizes calculated on a volume basis, representing the cumulative percentage from the smaller particle size side when D10 is 10% and when D90 is 90%.

[0046] A flame is formed by mixing a combustible gas with an oxygen-containing combustion-supporting gas and causing it to burn. The temperature of the furnace's refractory structure, as an indicator of the furnace temperature, is between 900°C and 1500°C at its highest point (furnace body temperature). As a lower limit for the furnace body temperature, 900°C, 1000°C, and 1100°C can be used; as an upper limit, 1500°C, 1400°C, and 1300°C can be used. These upper and lower limits can be combined arbitrarily. Air or oxygen can be used as the combustion-supporting gas. The combustible gas and the combustion-supporting gas can be supplied to the furnace separately or in a pre-mixed state. In the case of separate supply, the combustible gas is supplied to the inner pipe of the double-layered tube, and the combustion-supporting gas is supplied to the outer pipe. The flow rate of the combustible gas is preferably 10 m / s or more, more preferably 15 m / s or more, and even more preferably 20 m / s or more. The flow rate of the combustion-supporting gas is preferably 10 m / s or more, more preferably 15 m / s or more, and even more preferably 20 m / s or more. The ratio of combustible gas to combustion-supporting gas, in terms of flow rate ratio, is preferably 2.0 or less, more preferably 1.5 or less, and even more preferably 1.0 or less. The supply amounts of combustible gas and combustion-supporting gas are the amount of combustible gas sufficient to form a flame large enough to sufficiently heat the supplied raw material particles, and the amount of combustion-supporting gas sufficient to fully combust the combustible gas. For example, the combustible gas content is 0.5 Nm³ relative to the unit weight of the processed raw material particles. 3 / kg~5Nm 3 / kg, so that the oxygen, as the combustion-supporting gas, is 1Nm³. 3 / kg~5Nm 3Approximately / kg. Then, in the case where the raw material contains metal particles (i.e., VMC method), an oxidizing flame is used as the flame.

[0047] Furthermore, it is preferable to supply air, such as sheath gas, around the flame. With sheath gas, the shape of the flame can be controlled and its influence on the furnace flame can be suppressed, and the obtained particle material can be rapidly cooled. The flow rate of the sheath gas, relative to the unit weight of the raw material particle material, can be 5 Nm³. 3 / kg, 20Nm 3 / kg, 40Nm 3 Approximately / kg. Additionally, the sheath gas inlet can be set to multiple sections, allowing for arbitrary adjustment of the flow rate according to height.

[0048] There are no particular limitations on the method of supplying raw material particles into the flame; they can be supplied to the flame in a dispersed state within a carrier gas. Examples of carrier gases include air, oxygen, and nitrogen.

[0049] The concentration of the raw material particles dispersed in the carrier gas is not particularly limited, but it is preferred to have a raw material particle concentration of 0.5 kg / Nm³. 3 ~8.0kg / Nm 3 Approximately, more preferably 1.0 kg / Nm 3 ~6.0kg / Nm 3 Approximately, and more preferably 1.5 kg / Nm 3 ~4.0kg / Nm 3 about.

[0050] The manufactured particulate material is recycled through classification using bag filters and cyclone separators.

[0051] The obtained particle material can be surface treated using the surface treatment agents described above.

[0052] (Semiconductor mounting material filler and semiconductor mounting material)

[0053] The semiconductor mounting material of this embodiment is a material formed by dispersing the semiconductor mounting material filler of this embodiment in a resin material. The filler for the semiconductor mounting material of this embodiment can be partially or entirely composed of the particulate material of this embodiment described above. The resin material is not particularly limited and can include, for example, epoxy resin, silicone resin, etc. A thermosetting resin prior to curing is particularly preferred. Based on the overall mass, the filler for the semiconductor mounting material preferably contains approximately 20% to 92% of the resin material, more preferably approximately 40% to 90%, and even more preferably approximately 60% to 88%.

[0054] Example

[0055] The following describes in detail the filler for semiconductor mounting materials and its manufacturing method, as well as the semiconductor mounting materials of the present invention, based on embodiments.

[0056] (Manufacturing of particle materials constituting fillers for semiconductor mounting materials)

[0057] • The raw material particles are crystalline and crushed silica, and the combustible gas is ammonia.

[0058] Example 1

[0059] Ammonia, a non-carbon-containing gas, is used as the flammable gas. Crystallized, crushed silica (silica A: volume average particle size 12.3 μm) is used as the raw material particle. Oxygen is used as the carrier gas.

[0060] The supply rate of silicon dioxide (A) is 20.2 kg / h, and the supply rate of ammonia is 32.1 Nm³. 3 / h, oxygen is used as a combustion-supporting gas, with a supply of 33.0 Nm³. 3 The obtained particle material was recovered using a cyclone separator and a bag filter, and used as the test sample in this embodiment.

[0061] Analysis of the obtained test samples showed a sphericity of 0.95 and four colored foreign objects larger than 20 μm. The volume average particle size of the obtained test samples was 15.6 μm. The melt density was 94.0%.

[0062] The amount of coloring foreign matter was determined using the method described in the embodiments. The coloring foreign matter was identified as containing carbon atoms by EDX, but since carbon atoms were not present in the raw material particles, combustible gas, combustion-supporting gas, carrier gas, etc., it was presumed that carbon-based particles originally present in the same embodiment had been mixed in. The same applies to Example 2 below. For the melt density of silicon dioxide, the peaks from crystalline materials and the halos from amorphous materials were separated based on the spectrum measured by XRD, and the proportion of amorphous material on a whole-body basis was used as the melt density based on their ratio. The melt density of alumina was calculated using the following formula.

[0063] (Melting point of alumina) = {1 - (S1 - S2) / (S3 - S2)} × 100 (%)

[0064] S1: BET specific surface area of ​​each test case

[0065] S2: Specific surface area (=6 / ρd) derived based on the particle size D50 value of each test example, assuming ideal spherical particles.

[0066] S3: BET specific surface area of ​​raw material particles

[0067] ρ: True density of aluminum oxide

[0068] d: Particle size D50 value of each test case

[0069] Example 2

[0070] The supply rate of silica A is set at 15.0 kg / h, and the supply rate of combustion-supporting gas is set at 28.0 Nm³. 3 / h, except that the particulate material is manufactured in the same manner as in Example 1.

[0071] Analysis of the obtained test samples showed a sphericity of 0.96 and the presence of three colored foreign matter particles larger than 20 μm. The volume average particle size of the obtained test samples was 14.3 μm. The melt density was 93.7%.

[0072] Example 3

[0073] The supply rate of silica A is set at 10.3 kg / h, and the supply rate of combustion-supporting gas is set at 28.0 Nm³. 3 / h, except that the particulate material is manufactured in the same manner as in Example 1.

[0074] Analysis of the obtained test samples showed a sphericity of 0.97 and zero colored foreign matter larger than 20 μm. The volume average particle size of the obtained test samples was 14.9 μm. The melt density was 96.7%.

[0075] • The raw material particles are crystalline and crushed silica; the combustible gases are ammonia and hydrogen.

[0076] Example 4

[0077] The supply rate of silica A is set at 9.8 kg / h, replacing the separate supply of ammonia, and the supply rate of ammonia is set at 25.7 Nm³. 3 The hydrogen supply rate is set at 8.6 Nm³ / h. 3 / h, set the supply rate of combustion-supporting gas to 28.0 Nm 3 / h, except that the particulate material is manufactured in the same manner as in Example 1.

[0078] Analysis of the obtained test samples showed a sphericity of 0.96 and zero colored foreign matter larger than 20 μm. The volume average particle size of the obtained test samples was 13.6 μm. The melt density was 94.0%.

[0079] Example 5

[0080] The supply rate of silicon dioxide (A) was set at 19.3 kg / h, and the supply rate of ammonia was set at 16.1 Nm³. 3 The hydrogen supply rate is set at 21.1 Nm³ / h. 3 / h, set the supply rate of combustion-supporting gas to 25.0 Nm 3 / h, except that the particulate material is manufactured in the same manner as in Example 4.

[0081] Analysis of the obtained test samples showed a sphericity of 0.96 and zero colored foreign matter larger than 20 μm. The volume average particle size of the obtained test samples was 15.4 μm. The melt density was 95.3%.

[0082] • The raw material particles are crystalline and crushed silica, and the combustible gas is propane.

[0083] Comparative Example 1

[0084] As a flammable gas, propane is used instead of ammonia, with the propane supply set at 5.0 Nm³. 3 / h, set the supply rate of combustion-supporting gas to 28.0 Nm 3 / h, except that the particulate material is manufactured in the same manner as in Example 1. It should be noted that the calorific value of the flame per unit mass of the raw material is the same as in Example 1.

[0085] Analysis of the obtained test samples showed a sphericity of 0.97 and 22 colored foreign particles larger than 20 μm. The volume average particle size of the obtained test samples was 15.1 μm. SEM-EDX analysis of the separated colored foreign particles revealed elements containing amorphous coal particles, predominantly composed of carbon (C) and containing oxygen (O), as well as particles believed to be a mixture of silica and coal, predominantly composed of oxygen (O) and containing silicon (Si) and carbon (C).

[0086] Comparative Example 2

[0087] The supply rate of silica A is set at 20.3 kg / h, and the supply rate of combustion-supporting gas is set at 25.0 Nm³. 3 / h, except that the particulate material was manufactured in the same manner as in Comparative Example 1.

[0088] Analysis of the obtained test samples showed a sphericity of 0.95 and 31 colored foreign particles larger than 20 μm. The volume average particle size of the obtained test samples was 14.8 μm.

[0089] • The raw material particles are crystalline and crushed silica (small particle size), and the combustible gas is ammonia.

[0090] Example 6

[0091] Crystallized broken silica (silica B) with a volume average particle size of 5.3 μm was used instead of silica A, and the supply rate of silica B was set to 10.0 kg / h. Otherwise, the particulate material was manufactured in the same manner as in Example 1.

[0092] Analysis of the obtained test samples showed a sphericity of 0.95 and the presence of three colored foreign matter particles larger than 20 μm. The volume average particle size of the obtained test samples was 6.5 μm. The melt density was 92.8%.

[0093] • The raw material particles are crystalline and crushed silica (small particle size), and the combustible gas is propane.

[0094] Comparative Example 3

[0095] The supply rate of silica B is set at 16.4 kg / h. As a combustible gas, propane is used instead of ammonia, and the propane supply rate is set at 5.0 Nm³. 3 / h, except that the particulate material is manufactured in the same manner as in Example 6.

[0096] Analysis of the obtained test samples showed a sphericity of 0.96 and 16 colored foreign particles larger than 20 μm. The volume average particle size of the obtained test samples was 6.4 μm. The melt density was 96.7%.

[0097] • The raw material particles are alumina, and the combustible gas is ammonia.

[0098] Example 7

[0099] Instead of silica A, crushed alumina (alumina A) with a volume average particle size of 57.6 μm was used, and the supply rate of alumina A was set to 10.0 kg / h. Otherwise, the particulate material was manufactured in the same manner as in Example 2.

[0100] Analysis of the obtained test samples showed a sphericity of 0.96 and five colored foreign objects larger than 20 μm. The volume average particle size of the obtained test samples was 35.9 μm. The melt density was 70.4%.

[0101] • The raw material particles are alumina, and the combustible gas is propane.

[0102] Comparative Example 4

[0103] The supply rate of alumina A is set at 16.4 kg / h. As a combustible gas, propane is used instead of ammonia, and the propane supply rate is set at 5.0 Nm³. 3 / h, except that the particulate material is manufactured in the same manner as in Example 7.

[0104] Analysis of the obtained test samples showed a sphericity of 0.96 and 19 colored foreign particles larger than 20 μm. The volume average particle size of the obtained test samples was 45.5 μm. The melt density was 76.2%.

[0105] • The raw material particles are crystalline and crushed silica, and the combustible gas is hydrogen.

[0106] Example 8

[0107] The supply rate of silicon dioxide A is set to 5.0 kg / h, and hydrogen is used instead of ammonia, with the hydrogen supply rate set to 48.5 Nm³. 3 / h, set the supply rate of combustion-supporting gas to 25.5 Nm 3 / h, except that the particulate material is manufactured in the same manner as in Example 1.

[0108] Analysis of the obtained test samples showed a sphericity of 0.97 and zero colored foreign matter larger than 20 μm. The volume average particle size of the obtained test samples was 14.8 μm. The melt density was 96.9%.

[0109] The results of each embodiment and comparative example are shown in Table 1. Unless otherwise specified, inconsistencies between the table and other sources herein shall be superseded by the table.

[0110] [Table 1]

[0111]

[0112] • Inspection

[0113] It can be seen that the test specimens of the embodiment using a carbon-free gas as the combustible gas had a very small amount of coloring foreign matter compared to the test specimens of the comparative example using propane containing carbon as the combustible gas. This is believed to be because using a carbon-free gas as the combustible gas prevents the formation of impurities composed of carbon.

[0114] It should be noted that in Examples 1 and 2, 5-7, the observed colored foreign matter also included particles with a particle size of less than 20 μm, but did not necessarily contain carbon. Regardless of whether it contained carbon, it can be inferred that it came from experimental facilities such as furnaces, bag filters, and cyclone separators, impurities in raw material particles, or particles formed by the deterioration of raw material particles.

Claims

1. A method for manufacturing a filler for semiconductor mounting materials, comprising a particle-containing filler dispersed in a resin material to form the semiconductor mounting material. The particle material is mainly composed of the following metal oxides: the supernatant containing carbon-containing foreign matter larger than 20 μm in the size of a dispersion prepared by dispersing 50 g in 400 mL of ethanol is irradiated with ultrasound at 38 kHz and 300 W for 20 minutes and allowed to stand for 24 hours contains less than 10 particles, the volume average particle size is 0.1 μm to 40 μm, and the sphericity is greater than 0.

85. The manufacturing method includes the following spheroidizing step: a raw material particle material, mainly composed of the metal contained in the metal oxide and / or the metal oxide, is fed into a flame for combustion and / or melting to form the particle material. The flame is obtained by burning a combustible gas, wherein the combustible gas contains more than 20% by volume of a non-carbon-containing combustible gas that does not contain carbon.

2. The method for manufacturing filler for semiconductor mounting materials according to claim 1, wherein, The raw material particles contain the metal oxide.

3. The method for manufacturing filler for semiconductor mounting materials according to claim 1 or 2, wherein, The combustible gas contains 100% of the non-carbon-containing gas.

4. A method for manufacturing filler for semiconductor mounting materials according to any one of claims 1 to 3, wherein, The non-carbon-containing gas is ammonia and / or hydrogen.

5. A method for manufacturing filler for semiconductor mounting materials according to any one of claims 1 to 4, wherein, The metal oxide is silicon dioxide.

6. A filler for semiconductor mounting materials, comprising a particle material, wherein the particle material is mainly composed of the following metal oxide: the supernatant containing carbon-containing colored foreign matter larger than 20 μm in the form of a dispersion prepared by dispersing 50 g in 400 mL of ethanol under ultrasonic waves at 38 kHz and 300 W for 20 minutes and then allowed to stand for 24 hours contains fewer than 10 particles, the volume average particle size is 0.1 μm to 40 μm, and the sphericity is 0.85 or higher; The semiconductor mounting material is formed by dispersing fillers in a resin material.

7. The filler for semiconductor mounting material according to claim 6, wherein, The metal oxide is silicon dioxide.

8. A semiconductor mounting material, comprising: The filler for semiconductor mounting material as described in claim 6 or 7, and The resin material in which the filler for the semiconductor mounting material is dispersed.

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