# US 2010/0168307 A1 · Modified perovskite complex oxide, method for producing the same and composite dielectric material > Agents: this data is available as JSON from the patentgrep API and MCP server — see https://patentgrep.com/llms.txt - Number: US 2010/0168307 A1 - Document ID: US20100168307A1 - Status: Published application - Kind: A1 - Application number: 12/523,867 - Filed: 2008-01-16 - Published: 2010-07-01 - Earliest claimed: 2007-01-18 - Assignees: Nippon Chemical Industrial Co., Ltd. - Inventors: Naoaki Narishige; Shinji Tanabe - Web page: https://patentgrep.com/patent/US20100168307A1 ## CPC - C01G 23/006: {Alkaline earth titanates} - C01G 23/00: Compounds of titanium {(preparation of Ti-compounds from ores or scraps C22B34/12)} - C01G 25/00: Compounds of zirconium - C04B 35/62675: {characterised by the treatment temperature} - C04B 35/62807: {Silica or silicates} - C04B 35/62821: {Titanium oxide} - C04B 35/62886: {by wet chemical techniques} - C04B 35/62894: {with more than one coating layer} - C09C 1/00: Treatment of specific inorganic materials other than fibrous fillers (tenebrescent materials C09K9/00; luminescent materials C09K11/00); Preparation of carbon black - C09C 1/36: Compounds of titanium {(C09C1/0009, C09C1/0015, C09C1/0078 take precedence)} - C01P 2002/34: perovskite-type (ABO3) - C01P 2006/12: Surface area - C04B 2235/3249: containing also titanium oxide or titanates, e.g. lead zirconate titanate (PZT) - C04B 2235/5409: expressed by specific surface values - C04B 2235/5445: submicron sized, i.e. from 0,1 to 1 micron - Y10T 428/2991: Coated - Y10T 428/2993: Silicic or refractory material containing [e.g., tungsten oxide, glass, cement, etc.] - Y10T 428/2995: Silane, siloxane or silicone coating - C01G: COMPOUNDS CONTAINING METALS NOT COVERED BY SUBCLASSES C01D OR C01F (metal hydrides {monoborane, diborane or addition complexes thereof} C01B6/00; salts of oxyacids of halogens C01B11/00; peroxides, salts or peroxyacids C01B15/00; thiosulfates, dithionites, polythionates C01B17/64; compounds containing selenium, or tellurium C01B19/00; binary compounds of nitrogen with metals C01B21/06; azides C01B21/08; {compounds containing nitrogen, other non-metals and metal C01B21/082}; metal amides C01B21/092; nitrites C01B21/50; {compounds of noble gases C01B23/0005}; phosphides C01B25/08; salts of oxyacids of phosphorus C01B25/16; carbides C01B32/90; compounds containing silicon C01B33/00; compounds containing boron C01B35/00; compounds having molecular sieve properties but not having base-exchange properties C01B37/00; compounds having molecular sieve and base-exchange properties, e.g. crystalline zeolites, C01B39/00; cyanides C01C3/08; salts of cyanamide C01C3/16; thiocyanates C01C3/20) - C04B: LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE {(roofing granules E04D7/005)}; CERAMICS (devitrified glass-ceramics C03C10/00); REFRACTORIES; TREATMENT OF NATURAL STONE - C09C: TREATMENT OF INORGANIC MATERIALS, OTHER THAN FIBROUS FILLERS, TO ENHANCE THEIR PIGMENTING OR FILLING PROPERTIES (treatment of materials specially adapted to enhance their filling properties in mortars, concrete or artificial stone C04B14/00, C04B18/00, C04B20/00); PREPARATION OF CARBON BLACK {; PREPARATION OF INORGANIC MATERIALS WHICH ARE NO SINGLE CHEMICAL COMPOUNDS AND WHICH ARE MAINLY USED AS PIGMENTS OR FILLERS} - C01P: INDEXING SCHEME RELATING TO STRUCTURAL AND PHYSICAL ASPECTS OF SOLID INORGANIC COMPOUNDS - Y10T: TECHNICAL SUBJECTS COVERED BY FORMER US CLASSIFICATION ## Abstract It is an object of the present invention to provide: a modified perovskite-type composite oxide, which effectively suppresses elution of A-site metals from a perovskite-type composite oxide, and which can be particularly preferably used as an inorganic filler for a composite dielectric body; a method for producing the same; and a composite dielectric material using the same. The modified perovskite-type composite oxide of the present invention is produced by primarily coating the particle surface of a perovskite-type composite oxide with silica and then secondarily coating it with a coupling agent, characterized in that the layer primarily coated with silica is produced by performing a heat treatment at 800° C. to 1200° C. on hydrolyzed silica obtained by the hydrolysis of tetraalkoxysilane. ## Claims ### Claim 1 A modified perovskite-type composite oxide, which is produced by primarily coating a particle surface of a perovskite-type composite oxide with a layer of silica and then secondarily coating the resultant particle surface with a coupling agent, wherein the layer primarily coated with silica is produced by performing a heat treatment at 800° C. to 1200° C. on hydrolyzed silica obtained by the hydrolysis of tetraalkoxysilane. ### Claim 2 (depends on 1) The modified perovskite-type composite oxide according to claim 1, wherein the modified perovskite-type composite oxide has pH 8.0 or less that is obtained by contact with water. ### Claim 3 (depends on 1) The modified perovskite-type composite oxide according to claim 1, wherein the amount of silica on the first coated layer per unit surface area of a substrate is 3×10−5 to 40×10−5 mol/m2. ### Claim 4 (depends on 1) The modified perovskite-type composite oxide according to claim 1, wherein the perovskite-type composite oxide primarily coated with silica has pH 8.0 or less that is obtained by contact with water. ### Claim 5 (depends on 1) The modified perovskite-type composite oxide according to claim 1, wherein the coupling agent is at least one selected from a silane coupling agent, an aluminum coupling agent, a titanate coupling agent, and a zirconate coupling agent. ### Claim 6 (depends on 1) The modified perovskite-type composite oxide according to claim 1, wherein the coating amount of the coupling agent is 0.04% to 5% by weight. ### Claim 7 (depends on 1) The modified perovskite-type composite oxide according to claim 1, wherein the modified perovskite-type composite oxide is of ABO3 type, and wherein A-site element is one or more selected from the group consisting of Ba, Ca, Sr, and Mg, and B-site element is one or two selected from the group consisting of Ti and Zr. ### Claim 8 (depends on 1) The modified perovskite-type composite oxide according to claim 1, wherein the modified perovskite-type composite oxide has a BET specific surface area of 0.5 to 12 m2/g. ### Claim 9 (depends on 1) The modified perovskite-type composite oxide according to claim 1, wherein the modified perovskite-type composite oxide is used as an inorganic filler. ### Claim 10 A method for producing a modified perovskite-type composite oxide, comprising the steps of: (A1) preparing a slurry comprising a perovskite-type composite oxide and a hydrophilic organic solvent; (A2) adding tetraalkoxysilane to the slurry, and carrying out a hydrolysis reaction in the presence of a catalyst to precipitate silica on the particle surface of the perovskite-type composite oxide, so as to obtain a perovskite-type composite oxide coated with the hydrolyzed silica; (A3) drying and then performing a heat treatment at 800° C. to 1200° C. on the perovskite-type composite oxide coated with the hydrolyzed silica, so as to obtain a perovskite-type composite oxide that is primarily coated with silica; and (A4) allowing the perovskite-type composite oxide that is primarily coated with silica to come into contact with a coupling agent. ### Claim 11 (depends on 10) The method for producing a modified perovskite-type composite oxide according to claim 10, wherein the perovskite-type composite oxide that is primarily coated with silica produced in step (A3) has pH 8.0 or less that is obtained by contact with water. ### Claim 12 A composite dielectric material, comprising: a modified perovskite-type composite oxide, which is produced by primarily coating a particle surface of a perovskite-type composite oxide with a layer of silica and then secondarily coating the resultant particle surface with a coupling agent, wherein the layer primarily coated with silica is produced by performing a heat treatment at 800° C. to 1200° C. on hydrolyzed silica obtained by the hydrolysis of tetraalkoxysilane, and the modified perovskite-type composite oxide is disposed in a polymeric material. ### Claim 13 (depends on 12) The composite dielectric material according to claim 12, wherein the composite dielectric material is used in electronic components. ### Claim 14 (depends on 12) The composite dielectric material according to claim 12, wherein the amount of silica on the first coated layer per unit surface area of a substrate is 3×10−5 to 40×10−5 mol/m2. ### Claim 15 (depends on 12) The composite dielectric material according to claim 12, wherein the coupling agent is at least one selected from a silane coupling agent, an aluminum coupling agent, a titanate coupling agent, and a zirconate coupling agent. ### Claim 16 (depends on 12) The composite dielectric material according to claim 12, wherein the coating amount of the coupling agent is 0.04% to 5% by weight. ### Claim 17 (depends on 12) The composite dielectric material according to claim 12, wherein the modified perovskite-type composite oxide is of ABO3 type, and wherein A-site element is one or more selected from the group consisting of Ba, Ca, Sr, and Mg, and B-site element is one or two selected from the group consisting of Ti and Zr. ### Claim 18 (depends on 12) The composite dielectric material according to claim 12, wherein the modified perovskite-type composite oxide has a BET specific surface area of 0.5 to 12 m2/g.