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WO2005033216A1 - Poudre d'oxyde de magnesium revetue comprenant une charge elevee et son procede de production, et composition de resine contenant ladite poudre - Google Patents

Poudre d'oxyde de magnesium revetue comprenant une charge elevee et son procede de production, et composition de resine contenant ladite poudre Download PDF

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Publication number
WO2005033216A1
WO2005033216A1 PCT/JP2003/015954 JP0315954W WO2005033216A1 WO 2005033216 A1 WO2005033216 A1 WO 2005033216A1 JP 0315954 W JP0315954 W JP 0315954W WO 2005033216 A1 WO2005033216 A1 WO 2005033216A1
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WO
WIPO (PCT)
Prior art keywords
magnesium oxide
powder
oxide powder
resin composition
resin
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Ceased
Application number
PCT/JP2003/015954
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English (en)
Japanese (ja)
Inventor
Toshio Kiyokawa
Kaori Yamamoto
Masaaki Kunishige
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Tateho Chemical Industries Co Ltd
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Tateho Chemical Industries Co Ltd
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Filing date
Publication date
Application filed by Tateho Chemical Industries Co Ltd filed Critical Tateho Chemical Industries Co Ltd
Priority to JP2005509330A priority Critical patent/JP4237182B2/ja
Priority to AU2003289060A priority patent/AU2003289060A1/en
Publication of WO2005033216A1 publication Critical patent/WO2005033216A1/fr
Anticipated expiration legal-status Critical
Ceased legal-status Critical Current

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Classifications

    • C—CHEMISTRY; METALLURGY
    • C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09C—TREATMENT OF INORGANIC MATERIALS, OTHER THAN FIBROUS FILLERS, TO ENHANCE THEIR PIGMENTING OR FILLING PROPERTIES ; PREPARATION OF CARBON BLACK  ; PREPARATION OF INORGANIC MATERIALS WHICH ARE NO SINGLE CHEMICAL COMPOUNDS AND WHICH ARE MAINLY USED AS PIGMENTS OR FILLERS
    • C09C1/00—Treatment of specific inorganic materials other than fibrous fillers; Preparation of carbon black
    • C09C1/02—Compounds of alkaline earth metals or magnesium
    • C09C1/028—Compounds containing only magnesium as metal
    • H—ELECTRICITY
    • H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
    • H05K—PRINTED CIRCUITS; CASINGS OR CONSTRUCTIONAL DETAILS OF ELECTRIC APPARATUS; MANUFACTURE OF ASSEMBLAGES OF ELECTRICAL COMPONENTS
    • H05K1/00—Printed circuits
    • H05K1/02—Details
    • H05K1/03—Use of materials for the substrate
    • H05K1/0313—Organic insulating material
    • H05K1/0353—Organic insulating material consisting of two or more materials, e.g. two or more polymers, polymer + filler, + reinforcement
    • H05K1/0373—Organic insulating material consisting of two or more materials, e.g. two or more polymers, polymer + filler, + reinforcement containing additives, e.g. fillers
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01P—INDEXING SCHEME RELATING TO STRUCTURAL AND PHYSICAL ASPECTS OF SOLID INORGANIC COMPOUNDS
    • C01P2004/00—Particle morphology
    • C01P2004/30—Particle morphology extending in three dimensions
    • C01P2004/32—Spheres
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01P—INDEXING SCHEME RELATING TO STRUCTURAL AND PHYSICAL ASPECTS OF SOLID INORGANIC COMPOUNDS
    • C01P2004/00—Particle morphology
    • C01P2004/80—Particles consisting of a mixture of two or more inorganic phases
    • C01P2004/82—Particles consisting of a mixture of two or more inorganic phases two phases having the same anion, e.g. both oxidic phases
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01P—INDEXING SCHEME RELATING TO STRUCTURAL AND PHYSICAL ASPECTS OF SOLID INORGANIC COMPOUNDS
    • C01P2004/00—Particle morphology
    • C01P2004/80—Particles consisting of a mixture of two or more inorganic phases
    • C01P2004/82—Particles consisting of a mixture of two or more inorganic phases two phases having the same anion, e.g. both oxidic phases
    • C01P2004/84—Particles consisting of a mixture of two or more inorganic phases two phases having the same anion, e.g. both oxidic phases one phase coated with the other
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01P—INDEXING SCHEME RELATING TO STRUCTURAL AND PHYSICAL ASPECTS OF SOLID INORGANIC COMPOUNDS
    • C01P2006/00—Physical properties of inorganic compounds
    • C01P2006/11—Powder tap density
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01P—INDEXING SCHEME RELATING TO STRUCTURAL AND PHYSICAL ASPECTS OF SOLID INORGANIC COMPOUNDS
    • C01P2006/00—Physical properties of inorganic compounds
    • C01P2006/12—Surface area
    • H—ELECTRICITY
    • H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
    • H05K—PRINTED CIRCUITS; CASINGS OR CONSTRUCTIONAL DETAILS OF ELECTRIC APPARATUS; MANUFACTURE OF ASSEMBLAGES OF ELECTRICAL COMPONENTS
    • H05K2201/00—Indexing scheme relating to printed circuits covered by H05K1/00
    • H05K2201/02—Fillers; Particles; Fibers; Reinforcement materials
    • H05K2201/0203—Fillers and particles
    • H05K2201/0206—Materials
    • H05K2201/0209—Inorganic, non-metallic particles

Definitions

  • the present invention relates to a highly-filled coated magnesium oxide powder and a resin composition containing the powder.
  • the present invention relates to a coated magnesium oxide powder excellent in moisture resistance and excellent in filling when used as a filler, and a resin composition excellent in fluidity containing the coated magnesium oxide powder.
  • Electronic devices are composed of electronic components such as laminates, printed wiring boards, and multilayer wiring boards.
  • a resin composition is usually used for a pre-preda, a spacer, a sealant, an adhesive sheet, and the like, and a resin composition is required to have various performances or characteristics.
  • recent trends include the mounting of high-capacity power elements and high-density mounting in electronic devices, and as a result, the resin composition and its applied products are required to have better heat dissipation and moisture resistance than before. ing.
  • silica silicon dioxide
  • alumina aluminum oxide
  • magnesium oxide which has an order of magnitude higher thermal conductivity than silica and about the same thermal conductivity as alumina, is being studied as a material for resin fillers for semiconductor encapsulation.
  • magnesium oxide powder has higher hygroscopicity than silica powder. Therefore, when magnesium oxide powder is used as a resin filler for semiconductor encapsulation, problems such as generation of cracks due to volume expansion of the filler and reduction of thermal conductivity due to hydration of the absorbed water and magnesium oxide. Had occurred. Therefore, it is necessary to provide moisture resistance to magnesium oxide powder used as a resin filler for semiconductor encapsulation. Has been a major issue in guaranteeing long-term stable operation of the.
  • JP-A-2003-34522 and JP-A-2003-34525 disclose aluminum salt or cake.
  • the magnesium compound powder is mixed with the magnesium oxide powder, the solid content is filtered off, dried, and calcined, so that the surface of the magnesium oxide powder is coated with a coating layer containing aluminum or a double oxide of silicon and magnesium.
  • a method for producing a coated magnesium oxide powder is disclosed.
  • the coated magnesium oxide powder obtained by these methods has improved moisture resistance, since the powder particles have an angular shape, the filling property of the resin is low, and the flow of the obtained resin composition is further reduced. There is a problem that the property is low.
  • Japanese Patent No. 2590491 discloses that alumina and / or sily particles are added to magnesium oxide powder, and this is granulated using a spray drier to obtain spherical granules. Thereafter, a method for producing a magnesium oxide-based material is disclosed in which at least a part of the granulated material is melted without breaking a strong granulated state, and then the granulated material is rapidly cooled.
  • This method aims at improving the moisture resistance of the magnesium oxide particles.However, since the particles are granulated using a spray drier, the obtained spherical granules are aggregates of particles, that is, porous materials, and are formed into resin. High filling is expected to be difficult.
  • An object of the present invention is to provide a coated magnesium oxide powder that solves the above-mentioned problems, has excellent moisture resistance, and has excellent filling properties when used as a filler, and can be highly filled into a resin.
  • Another object of the present invention is to provide a resin composition containing the coated magnesium oxide powder and having excellent moisture resistance, thermal conductivity and fluidity, and an electronic device using the resin composition. Disclosure of the invention
  • the present inventor focused on the angle of repose as a parameter indicating the fluidity of the powder, and the tap density as a parameter indicating the filling property, while conducting various studies. Excellent flowability and filling when within a certain range It has been found that a powder having excellent flowability can be obtained by using the powder.
  • the surface is covered with the double oxide, oxide coated magnetic Shiumu powder repose angle of 5 5 degrees or less, and the tap density is equal to or is 1. 6 5 g / m 1 or more Is provided.
  • the coated magnesium oxide powder in the present invention has a surface coated with a double oxide, an angle of repose of 55 degrees or less, and a tap density of 1.65 g Zm 1 or more.
  • the angle of repose is one of the characteristic values for calculating the fluidity index of so-called Carr, which is an index for comprehensively evaluating the fluidity of powder proposed by R.L.Carr.
  • the fluidity of the powder can be evaluated by the angle of repose. Specifically, it refers to the angle between the generatrix and the horizontal plane of the cone formed when the powder is gently dropped on a horizontal surface using a funnel.
  • This angle of repose is preferably 50 degrees or less.
  • the tap density is an index for evaluating the filling property of powder, and refers to the mass of powder per unit volume when a powder sample is placed in a container of known volume and tapped a specified number of times from a certain height.
  • the tapping density is 1.65 g 1 or more, and more preferably 1.80 g / m 1 or more.
  • the surface of the coated magnesium oxide powder of the present invention is coated with a double oxide.
  • the composite oxide covering the surface of the magnesium oxide powder preferably contains magnesium and one or more elements selected from the group consisting of aluminum, iron, silicon and titanium.
  • the content of the double oxide used in the present invention is preferably from 5 to 50 mass%, more preferably from 10 to 40 mass%.
  • the content of the double oxide is within the above range, the surface of the magnesium oxide powder is completely covered with the double oxide, so that the moisture resistance is greatly improved, and the thermal conductivity of the resin composition after filling is further improved. It is also high, and can exhibit sufficient effects as a thermal conductive filler.
  • the average particle diameter of the coated magnesium oxide powder of the present invention is preferably 5 X 1 0- 6 ⁇ 5 0 0 X 10- 6 m, 10 X 10-6 ⁇ : I 00 X 10 one 6 m is more preferable. Further, the BET specific surface area is preferably 5.0 X 10 3 m 2 / kg or less, more preferably 1 X 10 3 m 2 // kg or less.
  • the coated magnesium oxide powder having a repose angle of 55 degrees or less and a tap density of 1.65 gZm 1 or more according to the present invention has a high temperature in the presence of a compound forming a double oxide on the surface of the magnesium oxide powder.
  • a compound forming a double oxide on the surface of the magnesium oxide powder By melting the coated magnesium oxide powder, it can be produced by spheroidizing the coated magnesium oxide powder. For example, powder is melted by passing it through a high-temperature flame, and spheroidized by surface tension.
  • the coated magnesium oxide powder obtained by this method is not always spherical, a powder satisfying the fluidity index and oil absorption of the present invention at the same time is produced by mixing powders having different particle diameters.
  • the compound used to form the double oxide is preferably at least one compound selected from the group consisting of an aluminum compound, an iron compound, a silicon compound and a titanium compound.
  • the form of the compound is not limited, but nitrates, sulfates, chlorides, oxynitrates, oxysulfates, oxychlorides, hydroxides and oxides are used.
  • the amount of these compounds in the magnesium oxide powder is finally obtained.
  • the content of the double oxide in the coated magnesium oxide powder is preferably determined to be 5 to 50 mass%.
  • Crystallite size of the magnesium oxide powder used in the present invention is preferably 5 0 X 1 0- 9 m or more. Crystallite diameter 5 0 X 1 0- 9 m or more oxidation Maguneshiu. Beam powder finer powder has low reactivity compared to, to uniformly adsorb Kei-containing compound or the like on the surface of the magnesium oxide powder Therefore, the composite oxide covering the surface of the magnesium oxide powder becomes uniform, and the water resistance is improved.
  • the crystallite diameter used in the present invention is a value calculated by the Scherrerr formula using the X-ray diffraction method.
  • one particle is a polycrystal composed of a plurality of single crystals, and the crystallite diameter indicates an average value of the size of the single crystal in the polycrystal.
  • the purity of the magnesium oxide powder is not particularly limited, and is preferably determined according to the application. For example, in order to satisfy the insulation properties of the electronic component, the purity is preferably 90% or more, and more preferably 95% or more.
  • the magnesium oxide powder having the characteristics of the present invention can be produced by a known method, for example, an electrofusion method or a sintering method. Resin composition containing coated magnesium oxide powder
  • a coated magnesium oxide powder having a high resin filling property can be easily obtained at low cost while maintaining moisture resistance and thermal conductivity. Further, the resin composition filled with the coated magnesium oxide powder thus obtained has good fluidity and improves moldability.
  • the resin composition of the present invention is obtained by adding the above-mentioned coated magnesium oxide powder to a resin.
  • the coated magnesium oxide powder of the present invention can be surface-treated with a silane-based coupling agent, a titanate-based coupling agent, or an aluminate-based coupling agent, if necessary, to further improve the filling property.
  • a silane-based coupling agent e.g., silane-based coupling agent, a titanate-based coupling agent, or an aluminate-based coupling agent, if necessary, to further improve the filling property.
  • silane coupling agent examples include vinyl trichlorosilane, vinyl oxysilane, glycidoxypropyl trialkoxysilane, methacryloxypropylmethyldialkoxysilane, and the like.
  • titanate-based coupling agents include isopropyltriisostearoyl titanate, tetraoctylbis (ditridecylphosphate) titanate, and bis (dioctylpyrophosphate).
  • the resin used in the resin composition of the present invention is not particularly limited, and is a thermosetting resin such as an epoxy resin, a phenol resin, a polyimide resin, a polyester resin, or a silicone resin, a polycarbonate resin, an acrylic resin, or a polyphenylene sulfide resin. And thermoplastic resins such as fluororesins. Of these, epoxy resins, silicone resins, and polyphenylene sulfide resins are preferred. If necessary, a curing agent and a curing accelerator can be added.
  • a thermosetting resin such as an epoxy resin, a phenol resin, a polyimide resin, a polyester resin, or a silicone resin, a polycarbonate resin, an acrylic resin, or a polyphenylene sulfide resin.
  • thermoplastic resins such as fluororesins.
  • epoxy resins, silicone resins, and polyphenylene sulfide resins are preferred. If necessary, a curing agent and a curing accelerator can be added.
  • Epoxy resins include bisphenol A epoxy resin, novolak epoxy resin, bisphenol F epoxy resin, brominated epoxy resin, orthocresol novolak epoxy resin, glycidyl ester resin, glycidylamine resin, and heterocyclic epoxy. Resins and the like.
  • phenol resin examples include novolak phenol resin and resole phenol resin.
  • silicone resin examples include a millable silicone rubber, a condensation type liquid silicone rubber, an addition type liquid silicone rubber, and a UV curing type silicone rubber, and the addition type liquid silicone rubber is preferable. Further, either one-pack type or two-pack type silicone rubber may be used, but two-pack type silicone rubber is preferable.
  • the resin composition of the present invention may contain a filler in addition to the above coated magnesium oxide powder.
  • the filler is not particularly limited, and examples thereof include fused silica and crystalline silica. If necessary, a release agent, a flame retardant, a coloring agent, a low stress imparting agent, and the like can be appropriately compounded.
  • the electronic device of the present invention uses the above resin composition for a part thereof, and has excellent heat dissipation and moisture resistance.
  • the electronic device include a resin circuit board, a metal base circuit board, a metal-clad laminate, and a metal-clad laminate with an inner circuit.
  • the resin composition of the present invention for the above electronic device include a semiconductor encapsulant, an adhesive or an adhesive sheet, a heat dissipation sheet, a heat dissipation spacer or a heat dissipation grease.
  • a paper base / glass substrate is immersed in the resin composition of the present invention, dried by heating and cured to a B stage, Resin cloth, resin paper, etc.
  • a resin circuit board, a metal-clad laminate, a metal-clad laminate with an inner layer circuit, and the like can be manufactured using this pre-preda.
  • a pre-preda is stacked according to the substrate thickness, a metal foil is placed, sandwiched between molds, inserted between hot plates of a press machine, and subjected to predetermined heating and pressing to form a laminate. Then, the four sides of the formed laminated board are cut, and the appearance is inspected to manufacture.
  • the resin composition of the present invention can be mixed with another base material and used as a base material in the form of a composite material such as glass epoxy or Teflon epoxy.
  • the resin composition of the present invention can be used as a sealing material.
  • the sealing resin is a resin material used for packaging for protecting the semiconductor chip from external factors such as mechanical, thermal stress and humidity. The performance of the formed package is indicated by the thermal conductivity and weather resistance of the cured resin.
  • the resin composition of the present invention can be used as an adhesive.
  • the adhesive refers to a substance used for bonding two objects, and the material of the adherend is not particularly limited.
  • the adhesive is temporarily given fluidity when applied or engaged on the surface of the adherend, and loses fluidity and solidifies after bonding.
  • a heat-sensitive adhesive such as a solvent adhesive, a pressure-sensitive adhesive, or an adhesive sheet, or a reactive adhesive can be used.
  • the resin composition of the present invention is used as an adhesive, the thermal conductivity and weather resistance after bonding are indicated by the thermal conductivity and weather resistance of the cured resin. -.
  • a metal-based circuit board can be manufactured by using the resin composition of the present invention as an adhesive.
  • the metal-based circuit board is manufactured by applying an adhesive on a metal plate, laminating metal foils when the adhesive is in the B-stage state, performing predetermined heating and pressing, and integrating them.
  • the resin composition of the present invention can be used as a heat dissipating material.
  • the heat dissipating material include a heat dissipating sheet, a heat dissipating spacer, and a heat dissipating grease.
  • the heat dissipation sheet is used to remove heat generated from heat-generating electronic components and electronic devices.
  • Air-insulating heat conductive sheet manufactured by filling silicone rubber with a heat conductive filler, and used mainly by attaching to heat radiating fins or metal plates.
  • the heat dissipation grease is the same as the heat dissipation sheet except that silicone oil is used instead of silicone rubber.
  • the heat-dissipating spacer is a thickness that fills the space between the heat-generating electronic components, the electronic device, and the case to directly transfer the heat generated from the heat-generating electronic components, the electronic device to the case of the electronic device.
  • Crystallite diameter 58. 3 X 1 0_ 9 assembly a is magnesium oxide Powder of single crystals of m to (Tateho Chemical Industries Co., Ltd. KMAO- H), using an impact-type dust ⁇ , particle size 100 X 1 It was ground to below 0- 6 m. Fumed silica (purity: 99.9% or more, specific surface area: 200 ⁇ 20 m 2 / g) is wet added to magnesium oxide so that the mixing ratio becomes 10 mass%, and the mixture is stirred at 400 to 500 rpm for 600 s. Mixed. After stirring and mixing, the cake obtained by filtration and dehydration was dried at 423 K using a dryer. The dried cake was crushed by a sample mill to adjust the particle size to about the same as the raw material magnesium oxide powder, to obtain a coated magnesium oxide powder.
  • X 1 0- 9 assembly a is magnesium oxide Powder of single crystals of m to (Tateho Chemical Industries Co., Ltd. KMAO- H), using an impact-type dust ⁇ , particle size 7 X 10-ground to less than 6 m. Fumed silica (purity: 99.9% or more, specific surface area: 200 ⁇ 2 Om 2 Zg) is wet added to magnesium oxide so that the mixing ratio becomes 10 mass%, and 600 at 400 to 500 rpm. The mixture was stirred and mixed. After stirring and mixing, the cake obtained by filtration and dehydration was dried at 423 K using a dryer. The dried cake was crushed by a sample mill to adjust the particle size to about the same as the raw material magnesium oxide powder, to obtain a coated magnesium oxide powder. Synthesis example 3
  • a coated magnesium oxide powder was obtained in the same manner as in Synthesis Example 1 except that the mixing ratio of the fumed silica force was 3 mass%.
  • a coated magnesium oxide powder was obtained in the same manner as in Synthesis Example 1 except that the mixing ratio of the fumed silica was 30 mAss%.
  • Crystallite diameter 58. 3 X 1 0- 9 assembly a is magnesium oxide Powder of single crystals of m to (Tateho Chemical Industries Co., Ltd. KMAO- H), using an impact-type dust ⁇ , particle size 1 00 X 10-ground to less than 6 m. 4% aqueous aluminum nitrate solution (manufactured by Kanto Chemical Co., Ltd. Ltd. special grade reagent), in terms of A 1 2 0 3, wet-added to the mixing ratio to magnesium oxide is 10 mass%, 400 to 500 rp For 600 s with stirring. After stirring and mixing, the mixture was filtered to form a cake.
  • the cake was sufficiently washed with water and dehydrated, and dried at 423 K using a dryer. Dried. The dried cake was crushed with a sample mill to adjust the particle size to about the same as the raw material magnesium oxide powder, to obtain a coated magnesium oxide powder.
  • iron nitrate aqueous solution in terms of F e 2 ⁇ 3, except that the mixing ratio against oxidation Ma Guneshiumu were blended so that 15 m ass%, in the same manner as in Synthesis Example 4 A coated magnesium oxide powder was obtained.
  • the powder prepared in Synthesis Example 1 was fed to a high temperature flame formed by burning of liquefied propane gas and oxygen, was melt-spheroidizing treatment was coated with false Terai Doo (Mg 2 S i 0 4) Spherical To obtain a coated magnesium oxide powder.
  • the powder produced in Synthesis Example 1 was calcined in air at 1723 K for 3600 s, and then re-crushed in a sample mill to adjust the particle size to the same level as the raw material magnesium oxide powder. (Mg 2 Si 0 4 ) coated magnesium oxide powder I got the end.
  • the powder prepared in Synthesis Example 2 was treated in the same manner as above to adjust the particle size to the same level as the raw material magnesium oxide powder, and coated with forsterite (Mg 2 Si 4 ). A coated magnesium oxide powder was obtained.
  • Example 3 The coated magnesium oxide powder obtained from Synthesis Example 1 and the coated magnesium oxide powder obtained from Synthesis Example 2 were mixed at a mass ratio of 7: 3.
  • Example 3 The coated magnesium oxide powder obtained from Synthesis Example 1 and the coated magnesium oxide powder obtained from Synthesis Example 2 were mixed at a mass ratio of 7: 3.
  • Example 5 Except for using the powder prepared in Synthesis Example 5 performs molten-spheroidizing treatment in the same manner as in Example 1 to obtain a coated oxide Maguneshiumu powder spherical coated with spinel (A 1 2 Mg 0 4) Was.
  • the powder obtained in Synthesis Example 1 was calcined in air at 1723 K for 3600 s, and then crushed again with a sample mill to adjust the particle size to about the same as the raw material magnesium oxide powder. (Mg 2 Si 4 ) to obtain a coated magnesium oxide powder.
  • Magnesium oxide powder is formed by combustion of liquefied propane gas and oxygen. The powder was supplied into a warm flame to obtain a magnesium oxide powder having an uncoated surface.
  • Angle of repose Using a powder property measurement device “Powder Tester PT-N” (manufactured by Hosokawa Micron Corporation), vibrating a standard sieve (opening 7 10 ⁇ ⁇ ) and dropping the powder sample through a funnel, using the injection method. The angle of repose (degree) was measured.
  • Tap density Using a powder property measurement device "Powder Tester I-II" (manufactured by Hosokawa Micron Corporation), put a powder sample in a 100 ml container, tap it 180 times from a certain height, and harden it with the impact of tapping. After that, the tapping density (g / ml) was measured.
  • Powder Tester I-II manufactured by Hosokawa Micron Corporation
  • BET specific surface area The specific surface area of the powder sample was measured by a gas adsorption method using a flow-type specific surface area measurement device “Flow Soap 1 1300” (manufactured by Shimadzu Corporation).
  • Average particle size Laser diffraction and scattering method
  • Example 3 Mg 2 Si0 4 6.56 50.7 1.747 20.24 0.54 4.12
  • Example 4 Mg 2 Si0 4 48.52 48.1 1.994 21.77 0.83 1.37
  • Example 5 Al 2 Mg0 4 21.76 47.4 1.701 20.45 0.78 2.77
  • Example 6 Fe 2 Mg0 4 21.00 48.2 1.840 20.21 0.31 1.08
  • Comparative Example 1 Mg 2 Si0 4 18.45 54.5 1.611 20.45 0.48 3.19 Comparative Example 2 ⁇ 1 46.4 1.930 21.09 0.81 7.34
  • Example 2 To the sample powder prepared in Example 1, 1.0 mass% of epoxysilane was added, and the powder was subjected to surface treatment by stirring and mixing for 600 s, and then dried at 420 K for 720 s. The obtained sample (560 parts by weight) was mixed with an ortho-cresol novolak epoxy resin.
  • the pellet was transfer molding with a 4 4 8 K in 1 8 0 s, 7 MP a , then performs a 1 8 X 1 0 3 s between Posutokiyua at 4 5 3 K, ⁇ 5 0 mm X t 3 mm Was obtained.
  • Example 7 Spiral flow was measured in the same manner as in Example 7 except that a mixed powder of coated magnesium oxide powders having different particle sizes prepared in Example 2 was used, and a molded product was obtained.
  • Example 6 Spiral flow was measured in the same manner as in Example 6 except that the spherical coated magnesium oxide powder produced in Example 5 was used, and a molded product was obtained.
  • Example 6 Except that the spherical coated magnesium oxide powder prepared in Example 6 was used Spiral flow was measured in the same manner as in Example 6 to obtain a molded body.
  • the spiral flow was measured in the same manner as in Example 7 except that the sample prepared in Comparative Example 1 was used, and a molded product was obtained.
  • Example 2 To the sample powder prepared in Example 1 was added 1.0% of butyltrimethoxysilane, and the mixture was stirred and mixed for 600 s to perform a surface treatment of the powder.
  • the viscosity was measured in the same manner as in Example 13 except that the mixed sample powder produced in Example 2 was used, and a molded product was obtained.
  • the viscosity was measured in the same manner as in Example 13 except that the sample powder produced in Comparative Example 1 was used, and a molded product was obtained.
  • the viscosity was measured in the same manner as in Example 13 except that the alumina powder was used instead of the magnesium oxide powder, to obtain a molded body.
  • Viscosity The viscosity was measured using a rheometer "VAR-50" (manufactured by REOLOG ICA), and the value of S hearrate was set to 1 s- 1 .
  • Thermal conductivity The thermal conductivity of the molded body was measured by a laser flash method using a thermal constant measuring device “TC 3000” (manufactured by Vacuum Riko Co., Ltd.).
  • Moisture resistance test The molded body was stored in a thermo-hygrostat set at a temperature of 358 K and a humidity of 85% for 7 days, and the moisture absorption was measured. The appearance was visually observed.
  • the coated magnesium oxide powder of the present invention that satisfies both the angle of repose and the tap density was subjected to a spheroidizing treatment (Table 1, Examples 1, 3 to 6) and fired. Both of those obtained by mixing the obtained powders (Table 1, Example 2) have excellent moisture resistance.
  • the resin composition filled with these powders (Table 2, Examples 7 to 14) has excellent fluidity, and the molded body has high thermal conductivity and moisture resistance. It was confirmed that it was excellent.
  • Comparative Example 1 was excellent in the moisture resistance, but the tap density was lower than the range of the present invention.
  • the fluidity was low when filled with epoxy resin (Table 2, Comparative Example 3) and when filled with silicone rubber (Table 2, Comparative Example 5).
  • the resin composition obtained by filling the conventional alumina powder in place of the magnesium oxide powder (Table 2, Comparative Examples 4 and 6) is excellent in fluidity and moisture resistance, but has poor thermal conductivity. Was inferior. Industrial applicability
  • the coated magnesium oxide powder of the present invention has excellent moisture resistance, and when used as a filler, has excellent filling properties, can be highly filled into a resin, and can be used as a heat conductive filler. Useful.
  • the resin composition obtained by filling the coated magnesium oxide powder has excellent fluidity, and the molded body has high heat dissipation and moisture resistance. It is very useful as a component material of a substrate, an adhesive or an adhesive sheet, a resin circuit board, a metal base circuit board, a metal-clad laminate, a metal-clad laminate with an inner layer circuit, etc., and its industrial value is extremely high. high.

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  • Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Engineering & Computer Science (AREA)
  • Microelectronics & Electronic Packaging (AREA)
  • Compounds Of Alkaline-Earth Elements, Aluminum Or Rare-Earth Metals (AREA)
  • Compositions Of Macromolecular Compounds (AREA)
  • Structures Or Materials For Encapsulating Or Coating Semiconductor Devices Or Solid State Devices (AREA)
  • Pigments, Carbon Blacks, Or Wood Stains (AREA)

Abstract

L'invention concerne une poudre d'oxyde de magnésium sphérique caractérisée en ce que sa surface est revêtue d'un oxyde double, et en ce qu'elle présente un angle de glissement de 55 degrés ou moins et une densité après tassement égale à 1,65 g/ml ou plus. L'invention concerne également une composition de résine comprenant ladite poudre et un dispositif électronique utilisant la composition de résine. La poudre d'oxyde de magnésium sphérique revêtue présente une excellente résistance à l'humidité ainsi qu'une excellente fluidité, et peut contenir une charge élevée en proportion lorsqu'on l'utilise comme charge dans une résine.
PCT/JP2003/015954 2003-10-03 2003-12-12 Poudre d'oxyde de magnesium revetue comprenant une charge elevee et son procede de production, et composition de resine contenant ladite poudre Ceased WO2005033216A1 (fr)

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JP2005509330A JP4237182B2 (ja) 2003-10-03 2003-12-12 高充填性被覆酸化マグネシウム粉末及びその粉末を含む樹脂組成物
AU2003289060A AU2003289060A1 (en) 2003-10-03 2003-12-12 Coated magnesium oxide powder capable of being highly filled and method for production thereof, and resin composition comprising the powder

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JP2003346085 2003-10-03
JP2003-346085 2003-10-03

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JP2006282783A (ja) * 2005-03-31 2006-10-19 Polyplastics Co 高熱伝導性樹脂組成物
JP2007045988A (ja) * 2005-08-12 2007-02-22 Tosoh Corp ポリアリーレンスルフィド組成物
JP2007045987A (ja) * 2005-08-12 2007-02-22 Tosoh Corp ポリアリーレンスルフィド系組成物
JP2007051270A (ja) * 2005-05-25 2007-03-01 Tosoh Corp ポリアリーレンスルフィド組成物
JP2007146105A (ja) * 2005-11-04 2007-06-14 Tosoh Corp ポリアリーレンスルフィド組成物
JP2007291300A (ja) * 2006-04-27 2007-11-08 Tosoh Corp ポリアリーレンスルフィド組成物
JP2007291220A (ja) * 2006-04-25 2007-11-08 Tosoh Corp ポリアリーレンスルフィド組成物
WO2011010291A1 (fr) * 2009-07-24 2011-01-27 Ticona Llc Compositions de polymère thermoconductrices et articles fabriqués à partir de celles-ci
JP2013035950A (ja) * 2011-08-09 2013-02-21 Tosoh Corp ポリアリーレンスルフィド樹脂組成物及びそれよりなる複合体
WO2013161844A1 (fr) * 2012-04-27 2013-10-31 ポリプラスチックス株式会社 Composition de résine ayant une conductivité thermique élevée
JP2017154937A (ja) * 2016-03-03 2017-09-07 株式会社大豊化成 熱伝導性複合フィラー、熱伝導性複合フィラーの製造方法、熱伝導性樹脂および熱伝導性樹脂の製造方法
WO2018056349A1 (fr) * 2016-09-21 2018-03-29 Dic株式会社 Particules de spinelle traitées en surface, son procédé de fabrication, composition de résine, et corps moulé
CN108017073A (zh) * 2017-12-27 2018-05-11 淮阴工学院 一种以水氯镁石为原料制备氧化镁气凝胶的方法
US20210317043A1 (en) * 2018-12-13 2021-10-14 Korea Institute Of Materials Science Magnesia, method for manufacturing same, highly thermally conductive magnesia composition, and magnesia ceramic using same

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JP7478631B2 (ja) * 2020-09-15 2024-05-07 デンカ株式会社 酸化マグネシウム粉末、フィラー組成物、樹脂組成物、及び放熱部品

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JPS6445716A (en) * 1987-08-14 1989-02-20 Asahi Glass Co Ltd Magnesium oxide powder
JPH02212314A (ja) * 1989-02-10 1990-08-23 Kyowa Chem Ind Co Ltd 高耐水和性、高流動性酸化マグネシウムの製造方法
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JP2003261796A (ja) * 2002-03-11 2003-09-19 Merck Ltd 体質顔料およびその製造方法

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JP2006282783A (ja) * 2005-03-31 2006-10-19 Polyplastics Co 高熱伝導性樹脂組成物
JP2007051270A (ja) * 2005-05-25 2007-03-01 Tosoh Corp ポリアリーレンスルフィド組成物
JP2007045988A (ja) * 2005-08-12 2007-02-22 Tosoh Corp ポリアリーレンスルフィド組成物
JP2007045987A (ja) * 2005-08-12 2007-02-22 Tosoh Corp ポリアリーレンスルフィド系組成物
US8357737B2 (en) 2005-11-04 2013-01-22 Tosoh Corporation Polyarylene sulfide composition
JP2007146105A (ja) * 2005-11-04 2007-06-14 Tosoh Corp ポリアリーレンスルフィド組成物
JP2007291220A (ja) * 2006-04-25 2007-11-08 Tosoh Corp ポリアリーレンスルフィド組成物
JP2007291300A (ja) * 2006-04-27 2007-11-08 Tosoh Corp ポリアリーレンスルフィド組成物
WO2011010291A1 (fr) * 2009-07-24 2011-01-27 Ticona Llc Compositions de polymère thermoconductrices et articles fabriqués à partir de celles-ci
JP2013035950A (ja) * 2011-08-09 2013-02-21 Tosoh Corp ポリアリーレンスルフィド樹脂組成物及びそれよりなる複合体
JPWO2013161844A1 (ja) * 2012-04-27 2015-12-24 ポリプラスチックス株式会社 高熱伝導性樹脂組成物
WO2013161844A1 (fr) * 2012-04-27 2013-10-31 ポリプラスチックス株式会社 Composition de résine ayant une conductivité thermique élevée
JP2017154937A (ja) * 2016-03-03 2017-09-07 株式会社大豊化成 熱伝導性複合フィラー、熱伝導性複合フィラーの製造方法、熱伝導性樹脂および熱伝導性樹脂の製造方法
WO2018056349A1 (fr) * 2016-09-21 2018-03-29 Dic株式会社 Particules de spinelle traitées en surface, son procédé de fabrication, composition de résine, et corps moulé
JPWO2018056349A1 (ja) * 2016-09-21 2019-09-05 Dic株式会社 表面処理スピネル粒子、その製造方法、樹脂組成物及び成形物
US11279830B2 (en) 2016-09-21 2022-03-22 Dic Corporation Surface-treated spinel particles, method for producing the same, resin composition, and molded article
CN108017073A (zh) * 2017-12-27 2018-05-11 淮阴工学院 一种以水氯镁石为原料制备氧化镁气凝胶的方法
CN108017073B (zh) * 2017-12-27 2019-08-23 淮阴工学院 一种以水氯镁石为原料制备氧化镁气凝胶的方法
US20210317043A1 (en) * 2018-12-13 2021-10-14 Korea Institute Of Materials Science Magnesia, method for manufacturing same, highly thermally conductive magnesia composition, and magnesia ceramic using same

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JPWO2005033216A1 (ja) 2006-12-14
AU2003289060A1 (en) 2005-04-21
JP4237182B2 (ja) 2009-03-11
TWI262897B (en) 2006-10-01

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