CN1323971C - 介电陶瓷制品前体和制备介电陶瓷制品的方法 - Google Patents
介电陶瓷制品前体和制备介电陶瓷制品的方法 Download PDFInfo
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- CN1323971C CN1323971C CNB038195135A CN03819513A CN1323971C CN 1323971 C CN1323971 C CN 1323971C CN B038195135 A CNB038195135 A CN B038195135A CN 03819513 A CN03819513 A CN 03819513A CN 1323971 C CN1323971 C CN 1323971C
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- zeolite
- ceramic article
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- 239000010457 zeolite Substances 0.000 title claims abstract description 101
- 239000000919 ceramic Substances 0.000 title claims abstract description 45
- HNPSIPDUKPIQMN-UHFFFAOYSA-N dioxosilane;oxo(oxoalumanyloxy)alumane Chemical compound O=[Si]=O.O=[Al]O[Al]=O HNPSIPDUKPIQMN-UHFFFAOYSA-N 0.000 claims abstract description 111
- 229910021536 Zeolite Inorganic materials 0.000 claims abstract description 98
- 239000000203 mixture Substances 0.000 claims abstract description 49
- 239000002243 precursor Substances 0.000 claims abstract description 29
- 239000000654 additive Substances 0.000 claims abstract description 20
- 229910044991 metal oxide Inorganic materials 0.000 claims abstract description 14
- 150000004706 metal oxides Chemical class 0.000 claims abstract description 14
- 229910000323 aluminium silicate Inorganic materials 0.000 claims abstract description 13
- 239000012702 metal oxide precursor Substances 0.000 claims abstract description 9
- 229910052751 metal Inorganic materials 0.000 claims abstract description 7
- 239000002184 metal Substances 0.000 claims abstract description 7
- ATJFFYVFTNAWJD-UHFFFAOYSA-N Tin Chemical compound [Sn] ATJFFYVFTNAWJD-UHFFFAOYSA-N 0.000 claims abstract description 4
- 238000000034 method Methods 0.000 claims description 21
- 230000000996 additive effect Effects 0.000 claims description 18
- 239000011777 magnesium Substances 0.000 claims description 18
- 229910052749 magnesium Inorganic materials 0.000 claims description 15
- 239000003795 chemical substances by application Substances 0.000 claims description 14
- FYYHWMGAXLPEAU-UHFFFAOYSA-N Magnesium Chemical compound [Mg] FYYHWMGAXLPEAU-UHFFFAOYSA-N 0.000 claims description 13
- -1 BaTiO 3 Inorganic materials 0.000 claims description 12
- 229910004298 SiO 2 Inorganic materials 0.000 claims description 12
- 239000013078 crystal Substances 0.000 claims description 10
- 229910052725 zinc Inorganic materials 0.000 claims description 10
- 239000011701 zinc Substances 0.000 claims description 10
- HCHKCACWOHOZIP-UHFFFAOYSA-N Zinc Chemical compound [Zn] HCHKCACWOHOZIP-UHFFFAOYSA-N 0.000 claims description 9
- JEWHCPOELGJVCB-UHFFFAOYSA-N aluminum;calcium;oxido-[oxido(oxo)silyl]oxy-oxosilane;potassium;sodium;tridecahydrate Chemical compound O.O.O.O.O.O.O.O.O.O.O.O.O.[Na].[Al].[K].[Ca].[O-][Si](=O)O[Si]([O-])=O JEWHCPOELGJVCB-UHFFFAOYSA-N 0.000 claims description 7
- 239000010955 niobium Substances 0.000 claims description 7
- 239000004902 Softening Agent Substances 0.000 claims description 6
- 229910052788 barium Inorganic materials 0.000 claims description 6
- 229910052791 calcium Inorganic materials 0.000 claims description 6
- 239000011575 calcium Substances 0.000 claims description 6
- 229910001690 harmotome Inorganic materials 0.000 claims description 6
- 229910001743 phillipsite Inorganic materials 0.000 claims description 6
- OYPRJOBELJOOCE-UHFFFAOYSA-N Calcium Chemical compound [Ca] OYPRJOBELJOOCE-UHFFFAOYSA-N 0.000 claims description 5
- ZOKXTWBITQBERF-UHFFFAOYSA-N Molybdenum Chemical compound [Mo] ZOKXTWBITQBERF-UHFFFAOYSA-N 0.000 claims description 5
- 229910002367 SrTiO Inorganic materials 0.000 claims description 5
- 229910010413 TiO 2 Inorganic materials 0.000 claims description 5
- 150000001342 alkaline earth metals Chemical class 0.000 claims description 5
- DSAJWYNOEDNPEQ-UHFFFAOYSA-N barium atom Chemical compound [Ba] DSAJWYNOEDNPEQ-UHFFFAOYSA-N 0.000 claims description 5
- 229910052728 basic metal Inorganic materials 0.000 claims description 5
- 150000003818 basic metals Chemical class 0.000 claims description 5
- 229910052750 molybdenum Inorganic materials 0.000 claims description 5
- 239000011733 molybdenum Substances 0.000 claims description 5
- 238000007493 shaping process Methods 0.000 claims description 5
- 229910052712 strontium Inorganic materials 0.000 claims description 5
- CIOAGBVUUVVLOB-UHFFFAOYSA-N strontium atom Chemical compound [Sr] CIOAGBVUUVVLOB-UHFFFAOYSA-N 0.000 claims description 5
- 229910052723 transition metal Inorganic materials 0.000 claims description 5
- 150000003624 transition metals Chemical class 0.000 claims description 5
- 229910006404 SnO 2 Inorganic materials 0.000 claims description 4
- 239000013543 active substance Substances 0.000 claims description 4
- 229910052784 alkaline earth metal Inorganic materials 0.000 claims description 4
- 150000001768 cations Chemical class 0.000 claims description 4
- 229910001723 mesolite Inorganic materials 0.000 claims description 4
- 229910052761 rare earth metal Inorganic materials 0.000 claims description 4
- 150000002910 rare earth metals Chemical class 0.000 claims description 4
- 239000010936 titanium Substances 0.000 claims description 4
- 229910052719 titanium Inorganic materials 0.000 claims description 4
- QTBSBXVTEAMEQO-UHFFFAOYSA-M Acetate Chemical compound CC([O-])=O QTBSBXVTEAMEQO-UHFFFAOYSA-M 0.000 claims description 3
- BVKZGUZCCUSVTD-UHFFFAOYSA-L Carbonate Chemical compound [O-]C([O-])=O BVKZGUZCCUSVTD-UHFFFAOYSA-L 0.000 claims description 3
- 229910052684 Cerium Inorganic materials 0.000 claims description 3
- KRKNYBCHXYNGOX-UHFFFAOYSA-K Citrate Chemical compound [O-]C(=O)CC(O)(CC([O-])=O)C([O-])=O KRKNYBCHXYNGOX-UHFFFAOYSA-K 0.000 claims description 3
- 229910002651 NO3 Inorganic materials 0.000 claims description 3
- NHNBFGGVMKEFGY-UHFFFAOYSA-N Nitrate Chemical compound [O-][N+]([O-])=O NHNBFGGVMKEFGY-UHFFFAOYSA-N 0.000 claims description 3
- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical compound [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 claims description 3
- QCWXUUIWCKQGHC-UHFFFAOYSA-N Zirconium Chemical compound [Zr] QCWXUUIWCKQGHC-UHFFFAOYSA-N 0.000 claims description 3
- 229910052787 antimony Inorganic materials 0.000 claims description 3
- WATWJIUSRGPENY-UHFFFAOYSA-N antimony atom Chemical compound [Sb] WATWJIUSRGPENY-UHFFFAOYSA-N 0.000 claims description 3
- 229910052758 niobium Inorganic materials 0.000 claims description 3
- GUCVJGMIXFAOAE-UHFFFAOYSA-N niobium atom Chemical compound [Nb] GUCVJGMIXFAOAE-UHFFFAOYSA-N 0.000 claims description 3
- 229910052715 tantalum Inorganic materials 0.000 claims description 3
- GUVRBAGPIYLISA-UHFFFAOYSA-N tantalum atom Chemical compound [Ta] GUVRBAGPIYLISA-UHFFFAOYSA-N 0.000 claims description 3
- 229910052718 tin Inorganic materials 0.000 claims description 3
- 229910052720 vanadium Inorganic materials 0.000 claims description 3
- 229910052726 zirconium Inorganic materials 0.000 claims description 3
- GWXLDORMOJMVQZ-UHFFFAOYSA-N cerium Chemical compound [Ce] GWXLDORMOJMVQZ-UHFFFAOYSA-N 0.000 claims 2
- LEONUFNNVUYDNQ-UHFFFAOYSA-N vanadium atom Chemical compound [V] LEONUFNNVUYDNQ-UHFFFAOYSA-N 0.000 claims 2
- 239000011521 glass Substances 0.000 abstract description 15
- 238000001354 calcination Methods 0.000 abstract description 11
- 239000011230 binding agent Substances 0.000 abstract description 4
- 229910052796 boron Inorganic materials 0.000 abstract description 2
- JKWMSGQKBLHBQQ-UHFFFAOYSA-N diboron trioxide Chemical compound O=BOB=O JKWMSGQKBLHBQQ-UHFFFAOYSA-N 0.000 abstract description 2
- 150000002739 metals Chemical class 0.000 abstract description 2
- 238000004519 manufacturing process Methods 0.000 abstract 2
- XOLBLPGZBRYERU-UHFFFAOYSA-N tin dioxide Chemical compound O=[Sn]=O XOLBLPGZBRYERU-UHFFFAOYSA-N 0.000 abstract 2
- 229910011255 B2O3 Inorganic materials 0.000 abstract 1
- ZOXJGFHDIHLPTG-UHFFFAOYSA-N Boron Chemical compound [B] ZOXJGFHDIHLPTG-UHFFFAOYSA-N 0.000 abstract 1
- 150000004649 carbonic acid derivatives Chemical class 0.000 abstract 1
- 150000002823 nitrates Chemical class 0.000 abstract 1
- 239000004014 plasticizer Substances 0.000 abstract 1
- 239000004094 surface-active agent Substances 0.000 abstract 1
- 238000005245 sintering Methods 0.000 description 14
- 239000000463 material Substances 0.000 description 8
- 239000000243 solution Substances 0.000 description 8
- 150000002500 ions Chemical class 0.000 description 7
- 239000000843 powder Substances 0.000 description 7
- 238000002360 preparation method Methods 0.000 description 7
- 239000011734 sodium Substances 0.000 description 7
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 6
- 239000004372 Polyvinyl alcohol Substances 0.000 description 5
- 229920001515 polyalkylene glycol Polymers 0.000 description 5
- 229920002451 polyvinyl alcohol Polymers 0.000 description 5
- 229910052708 sodium Inorganic materials 0.000 description 5
- 235000008733 Citrus aurantifolia Nutrition 0.000 description 4
- DGAQECJNVWCQMB-PUAWFVPOSA-M Ilexoside XXIX Chemical compound C[C@@H]1CC[C@@]2(CC[C@@]3(C(=CC[C@H]4[C@]3(CC[C@@H]5[C@@]4(CC[C@@H](C5(C)C)OS(=O)(=O)[O-])C)C)[C@@H]2[C@]1(C)O)C)C(=O)O[C@H]6[C@@H]([C@H]([C@@H]([C@H](O6)CO)O)O)O.[Na+] DGAQECJNVWCQMB-PUAWFVPOSA-M 0.000 description 4
- 235000011941 Tilia x europaea Nutrition 0.000 description 4
- 238000005516 engineering process Methods 0.000 description 4
- 239000010433 feldspar Substances 0.000 description 4
- 238000005342 ion exchange Methods 0.000 description 4
- 239000004571 lime Substances 0.000 description 4
- YIXJRHPUWRPCBB-UHFFFAOYSA-N magnesium nitrate Chemical compound [Mg+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O YIXJRHPUWRPCBB-UHFFFAOYSA-N 0.000 description 4
- ZWEHNKRNPOVVGH-UHFFFAOYSA-N 2-Butanone Chemical compound CCC(C)=O ZWEHNKRNPOVVGH-UHFFFAOYSA-N 0.000 description 3
- CSCPPACGZOOCGX-UHFFFAOYSA-N Acetone Chemical compound CC(C)=O CSCPPACGZOOCGX-UHFFFAOYSA-N 0.000 description 3
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 description 3
- PEDCQBHIVMGVHV-UHFFFAOYSA-N Glycerine Chemical compound OCC(O)CO PEDCQBHIVMGVHV-UHFFFAOYSA-N 0.000 description 3
- OKKJLVBELUTLKV-UHFFFAOYSA-N Methanol Chemical compound OC OKKJLVBELUTLKV-UHFFFAOYSA-N 0.000 description 3
- BQCADISMDOOEFD-UHFFFAOYSA-N Silver Chemical compound [Ag] BQCADISMDOOEFD-UHFFFAOYSA-N 0.000 description 3
- FKNQFGJONOIPTF-UHFFFAOYSA-N Sodium cation Chemical compound [Na+] FKNQFGJONOIPTF-UHFFFAOYSA-N 0.000 description 3
- HEMHJVSKTPXQMS-UHFFFAOYSA-M Sodium hydroxide Chemical compound [OH-].[Na+] HEMHJVSKTPXQMS-UHFFFAOYSA-M 0.000 description 3
- YXFVVABEGXRONW-UHFFFAOYSA-N Toluene Chemical compound CC1=CC=CC=C1 YXFVVABEGXRONW-UHFFFAOYSA-N 0.000 description 3
- 230000008901 benefit Effects 0.000 description 3
- 239000012700 ceramic precursor Substances 0.000 description 3
- KRKNYBCHXYNGOX-UHFFFAOYSA-N citric acid Chemical compound OC(=O)CC(O)(C(O)=O)CC(O)=O KRKNYBCHXYNGOX-UHFFFAOYSA-N 0.000 description 3
- 238000002425 crystallisation Methods 0.000 description 3
- 230000008025 crystallization Effects 0.000 description 3
- 239000002241 glass-ceramic Substances 0.000 description 3
- 238000010438 heat treatment Methods 0.000 description 3
- 239000003960 organic solvent Substances 0.000 description 3
- TWNQGVIAIRXVLR-UHFFFAOYSA-N oxo(oxoalumanyloxy)alumane Chemical compound O=[Al]O[Al]=O TWNQGVIAIRXVLR-UHFFFAOYSA-N 0.000 description 3
- 229910052700 potassium Inorganic materials 0.000 description 3
- 230000008569 process Effects 0.000 description 3
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N silicon dioxide Inorganic materials O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 3
- 229910052709 silver Inorganic materials 0.000 description 3
- 239000004332 silver Substances 0.000 description 3
- 239000002002 slurry Substances 0.000 description 3
- 239000002904 solvent Substances 0.000 description 3
- 239000000126 substance Substances 0.000 description 3
- 229910052721 tungsten Inorganic materials 0.000 description 3
- IRIAEXORFWYRCZ-UHFFFAOYSA-N Butylbenzyl phthalate Chemical compound CCCCOC(=O)C1=CC=CC=C1C(=O)OCC1=CC=CC=C1 IRIAEXORFWYRCZ-UHFFFAOYSA-N 0.000 description 2
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 description 2
- MQIUGAXCHLFZKX-UHFFFAOYSA-N Di-n-octyl phthalate Natural products CCCCCCCCOC(=O)C1=CC=CC=C1C(=O)OCCCCCCCC MQIUGAXCHLFZKX-UHFFFAOYSA-N 0.000 description 2
- LYCAIKOWRPUZTN-UHFFFAOYSA-N Ethylene glycol Chemical compound OCCO LYCAIKOWRPUZTN-UHFFFAOYSA-N 0.000 description 2
- CTQNGGLPUBDAKN-UHFFFAOYSA-N O-Xylene Chemical compound CC1=CC=CC=C1C CTQNGGLPUBDAKN-UHFFFAOYSA-N 0.000 description 2
- ZLMJMSJWJFRBEC-UHFFFAOYSA-N Potassium Chemical group [K] ZLMJMSJWJFRBEC-UHFFFAOYSA-N 0.000 description 2
- 239000007864 aqueous solution Substances 0.000 description 2
- 239000012298 atmosphere Substances 0.000 description 2
- 238000000498 ball milling Methods 0.000 description 2
- 230000015572 biosynthetic process Effects 0.000 description 2
- BJQHLKABXJIVAM-UHFFFAOYSA-N bis(2-ethylhexyl) phthalate Chemical compound CCCCC(CC)COC(=O)C1=CC=CC=C1C(=O)OCC(CC)CCCC BJQHLKABXJIVAM-UHFFFAOYSA-N 0.000 description 2
- 125000002091 cationic group Chemical group 0.000 description 2
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- 229910052802 copper Inorganic materials 0.000 description 2
- 239000010949 copper Substances 0.000 description 2
- JQVDAXLFBXTEQA-UHFFFAOYSA-N dibutylamine Chemical compound CCCCNCCCC JQVDAXLFBXTEQA-UHFFFAOYSA-N 0.000 description 2
- 150000002148 esters Chemical class 0.000 description 2
- 238000002474 experimental method Methods 0.000 description 2
- 230000001590 oxidative effect Effects 0.000 description 2
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical compound [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 description 2
- 239000011591 potassium Substances 0.000 description 2
- 238000010992 reflux Methods 0.000 description 2
- 238000003756 stirring Methods 0.000 description 2
- 239000000758 substrate Substances 0.000 description 2
- WFKWXMTUELFFGS-UHFFFAOYSA-N tungsten Chemical compound [W] WFKWXMTUELFFGS-UHFFFAOYSA-N 0.000 description 2
- 239000010937 tungsten Substances 0.000 description 2
- WRIDQFICGBMAFQ-UHFFFAOYSA-N (E)-8-Octadecenoic acid Natural products CCCCCCCCCC=CCCCCCCC(O)=O WRIDQFICGBMAFQ-UHFFFAOYSA-N 0.000 description 1
- QMMJWQMCMRUYTG-UHFFFAOYSA-N 1,2,4,5-tetrachloro-3-(trifluoromethyl)benzene Chemical compound FC(F)(F)C1=C(Cl)C(Cl)=CC(Cl)=C1Cl QMMJWQMCMRUYTG-UHFFFAOYSA-N 0.000 description 1
- PMOTYADHFATPGX-UHFFFAOYSA-N 1-phenylpropane-1-sulfonamide Chemical compound CCC(S(N)(=O)=O)C1=CC=CC=C1 PMOTYADHFATPGX-UHFFFAOYSA-N 0.000 description 1
- OVSKIKFHRZPJSS-UHFFFAOYSA-N 2,4-D Chemical compound OC(=O)COC1=CC=C(Cl)C=C1Cl OVSKIKFHRZPJSS-UHFFFAOYSA-N 0.000 description 1
- LQJBNNIYVWPHFW-UHFFFAOYSA-N 20:1omega9c fatty acid Natural products CCCCCCCCCCC=CCCCCCCCC(O)=O LQJBNNIYVWPHFW-UHFFFAOYSA-N 0.000 description 1
- QSBYPNXLFMSGKH-UHFFFAOYSA-N 9-Heptadecensaeure Natural products CCCCCCCC=CCCCCCCCC(O)=O QSBYPNXLFMSGKH-UHFFFAOYSA-N 0.000 description 1
- 229910017090 AlO 2 Inorganic materials 0.000 description 1
- 229920000742 Cotton Polymers 0.000 description 1
- 239000001856 Ethyl cellulose Substances 0.000 description 1
- ZZSNKZQZMQGXPY-UHFFFAOYSA-N Ethyl cellulose Chemical compound CCOCC1OC(OC)C(OCC)C(OCC)C1OC1C(O)C(O)C(OC)C(CO)O1 ZZSNKZQZMQGXPY-UHFFFAOYSA-N 0.000 description 1
- IAYPIBMASNFSPL-UHFFFAOYSA-N Ethylene oxide Chemical compound C1CO1 IAYPIBMASNFSPL-UHFFFAOYSA-N 0.000 description 1
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- 239000004166 Lanolin Substances 0.000 description 1
- OYHQOLUKZRVURQ-HZJYTTRNSA-N Linoleic acid Chemical compound CCCCC\C=C/C\C=C/CCCCCCCC(O)=O OYHQOLUKZRVURQ-HZJYTTRNSA-N 0.000 description 1
- JLVVSXFLKOJNIY-UHFFFAOYSA-N Magnesium ion Chemical compound [Mg+2] JLVVSXFLKOJNIY-UHFFFAOYSA-N 0.000 description 1
- 239000005642 Oleic acid Substances 0.000 description 1
- ZQPPMHVWECSIRJ-UHFFFAOYSA-N Oleic acid Natural products CCCCCCCCC=CCCCCCCCC(O)=O ZQPPMHVWECSIRJ-UHFFFAOYSA-N 0.000 description 1
- BPQQTUXANYXVAA-UHFFFAOYSA-N Orthosilicate Chemical compound [O-][Si]([O-])([O-])[O-] BPQQTUXANYXVAA-UHFFFAOYSA-N 0.000 description 1
- 229920003171 Poly (ethylene oxide) Polymers 0.000 description 1
- 239000004698 Polyethylene Substances 0.000 description 1
- 229920002367 Polyisobutene Polymers 0.000 description 1
- 235000021355 Stearic acid Nutrition 0.000 description 1
- BAECOWNUKCLBPZ-HIUWNOOHSA-N Triolein Natural products O([C@H](OCC(=O)CCCCCCC/C=C\CCCCCCCC)COC(=O)CCCCCCC/C=C\CCCCCCCC)C(=O)CCCCCCC/C=C\CCCCCCCC BAECOWNUKCLBPZ-HIUWNOOHSA-N 0.000 description 1
- PHYFQTYBJUILEZ-UHFFFAOYSA-N Trioleoylglycerol Natural products CCCCCCCCC=CCCCCCCCC(=O)OCC(OC(=O)CCCCCCCC=CCCCCCCCC)COC(=O)CCCCCCCC=CCCCCCCCC PHYFQTYBJUILEZ-UHFFFAOYSA-N 0.000 description 1
- 238000002441 X-ray diffraction Methods 0.000 description 1
- 238000010521 absorption reaction Methods 0.000 description 1
- DHKHKXVYLBGOIT-UHFFFAOYSA-N acetaldehyde Diethyl Acetal Natural products CCOC(C)OCC DHKHKXVYLBGOIT-UHFFFAOYSA-N 0.000 description 1
- 150000001241 acetals Chemical class 0.000 description 1
- XYLMUPLGERFSHI-UHFFFAOYSA-N alpha-Methylstyrene Chemical compound CC(=C)C1=CC=CC=C1 XYLMUPLGERFSHI-UHFFFAOYSA-N 0.000 description 1
- ANBBXQWFNXMHLD-UHFFFAOYSA-N aluminum;sodium;oxygen(2-) Chemical compound [O-2].[O-2].[Na+].[Al+3] ANBBXQWFNXMHLD-UHFFFAOYSA-N 0.000 description 1
- 229940070337 ammonium silicofluoride Drugs 0.000 description 1
- JXLHNMVSKXFWAO-UHFFFAOYSA-N azane;7-fluoro-2,1,3-benzoxadiazole-4-sulfonic acid Chemical compound N.OS(=O)(=O)C1=CC=C(F)C2=NON=C12 JXLHNMVSKXFWAO-UHFFFAOYSA-N 0.000 description 1
- UXXXZMDJQLPQPH-UHFFFAOYSA-N bis(2-methylpropyl) carbonate Chemical compound CC(C)COC(=O)OCC(C)C UXXXZMDJQLPQPH-UHFFFAOYSA-N 0.000 description 1
- 239000005385 borate glass Substances 0.000 description 1
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- 229910052792 caesium Inorganic materials 0.000 description 1
- TVFDJXOCXUVLDH-UHFFFAOYSA-N caesium atom Chemical group [Cs] TVFDJXOCXUVLDH-UHFFFAOYSA-N 0.000 description 1
- NWXHSRDXUJENGJ-UHFFFAOYSA-N calcium;magnesium;dioxido(oxo)silane Chemical compound [Mg+2].[Ca+2].[O-][Si]([O-])=O.[O-][Si]([O-])=O NWXHSRDXUJENGJ-UHFFFAOYSA-N 0.000 description 1
- ZMIGMASIKSOYAM-UHFFFAOYSA-N cerium Chemical compound [Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce] ZMIGMASIKSOYAM-UHFFFAOYSA-N 0.000 description 1
- 239000003153 chemical reaction reagent Substances 0.000 description 1
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- 230000002939 deleterious effect Effects 0.000 description 1
- DOIRQSBPFJWKBE-UHFFFAOYSA-N dibutyl phthalate Chemical compound CCCCOC(=O)C1=CC=CC=C1C(=O)OCCCC DOIRQSBPFJWKBE-UHFFFAOYSA-N 0.000 description 1
- 235000014113 dietary fatty acids Nutrition 0.000 description 1
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- JSKIRARMQDRGJZ-UHFFFAOYSA-N dimagnesium dioxido-bis[(1-oxido-3-oxo-2,4,6,8,9-pentaoxa-1,3-disila-5,7-dialuminabicyclo[3.3.1]nonan-7-yl)oxy]silane Chemical compound [Mg++].[Mg++].[O-][Si]([O-])(O[Al]1O[Al]2O[Si](=O)O[Si]([O-])(O1)O2)O[Al]1O[Al]2O[Si](=O)O[Si]([O-])(O1)O2 JSKIRARMQDRGJZ-UHFFFAOYSA-N 0.000 description 1
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- 150000004665 fatty acids Chemical class 0.000 description 1
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- 238000001914 filtration Methods 0.000 description 1
- 239000002223 garnet Substances 0.000 description 1
- PCHJSUWPFVWCPO-UHFFFAOYSA-N gold Chemical compound [Au] PCHJSUWPFVWCPO-UHFFFAOYSA-N 0.000 description 1
- 229910052737 gold Inorganic materials 0.000 description 1
- 239000010931 gold Substances 0.000 description 1
- 238000000227 grinding Methods 0.000 description 1
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- WGCNASOHLSPBMP-UHFFFAOYSA-N hydroxyacetaldehyde Natural products OCC=O WGCNASOHLSPBMP-UHFFFAOYSA-N 0.000 description 1
- 229910000765 intermetallic Inorganic materials 0.000 description 1
- 229920000831 ionic polymer Polymers 0.000 description 1
- QXJSBBXBKPUZAA-UHFFFAOYSA-N isooleic acid Natural products CCCCCCCC=CCCCCCCCCC(O)=O QXJSBBXBKPUZAA-UHFFFAOYSA-N 0.000 description 1
- 229940039717 lanolin Drugs 0.000 description 1
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- 229910052744 lithium Inorganic materials 0.000 description 1
- 238000011068 loading method Methods 0.000 description 1
- VTHJTEIRLNZDEV-UHFFFAOYSA-L magnesium dihydroxide Chemical compound [OH-].[OH-].[Mg+2] VTHJTEIRLNZDEV-UHFFFAOYSA-L 0.000 description 1
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Abstract
提出了一种介电陶瓷制品前体和一种制备介电陶瓷制品的方法。该陶瓷制品前体含有结晶硅铝酸盐沸石或无定形硅铝酸盐和玻璃相。该陶瓷制品前体可以非必要地含有至少一种选自由粘合剂、增塑剂和表面活性剂组成的组的成形助剂。该陶瓷制品前体中还可以含有B2O3或SnO2之类的金属氧化物添加剂以及硼或锡之类的金属的硝酸盐或碳酸盐之类的金属氧化物前体添加剂。制备介电陶瓷制品的方法包括将上述成分的混合物制成带材之类的成形制品，然后在700℃至1000℃的温度下将该成形制品煅烧0.5至24小时。
Description
发明背景
本发明涉及一种介电陶瓷制品前体和制备介电陶瓷制品的方法。该前体制品含有与玻璃相结合的结晶沸石或无定形硅铝酸盐。
对更小的多功能电子器件，例如具有互联网接入的无线电话、PDA等的需求使得多层电路的密度必须越来越高。这些多层电路通常使用充当绝缘衬底的电介质材料，在该衬底上沉积导电金属以形成布线层。
很早以来，氧化铝是所选的电介质材料，由于其高烧结温度(1400℃-1500℃)，就要求必须使用钨或钼之类的金属。然而，由于信号传输速度已经提高到1GHz及以上，钨或钼因其高电阻率已经不能使用。这就要求使用金、银或铜之类具有较低电阻率的金属。然而，这些金属的熔点低得多，这反过来要求使用在低至900℃的温度下烧结的电介质。
已经尝试使用低温共烧陶瓷(LTCC)的技术来满足这一需要。这些陶瓷是通过将玻璃质材料与晶相混合形成的。例如，US-A-5,821,181公开了制成氧化铝、玻璃质前体材料和改性剂的混合物。玻璃质材料含有SiO2、B2O3；MgO、CaO、SrO和BaO中的至少一种；以及K2O、Na2O和Li2O中的至少一种；而改性剂选自TiO2、SrTiO3和CaTiO3。US-A-4,714,687公开了制备含硅锌矿作为晶相的玻璃-陶瓷。该玻璃-陶瓷体含有ZnO、MgO、Al2O3和SiO2。US-A-5,164,342公开了含CaO、B2O3和SiO2的低介电玻璃陶瓷。在US-A-6,232,251 B1中，公开的介电陶瓷含有透辉石氧化物结晶相；选自石英结晶相和含Ti和Mg或Zn的复合氧化物结晶相的一种结晶相和玻璃相。
文献中还公开了可以将沸石组合物直接烧结成陶瓷。例如，US-A-5,071,801公开了由钾、铯或铷交换的沸石制备高密度的白榴石基陶瓷。该沸石中SiO2/Al2O3的比率为3.5/7.5。类似地，US-A-4,980,323和US-A-5,064,790公开了一种方法和由此方法制成的堇青石陶瓷。由Mg交换的沸石，例如沸石B、钙十字石、交沸石、水钙沸石、沸石ZK-19和沸石W，可以制备堇青石。此外，US-A-5,036,030公开了一种由SiO2/Al2O3比率不高于3.0的碱土金属形式的沸石和硼化合物(例如氧化硼)的混合物制备碱土金属硅铝酸盐烧结体的方法。最后，US-A-5,166,107公开了由SiO2/Al2O3比率低于3.0的钙型沸石制备钙长石烧结体。
与这一技术不同的是，申请人已经由结晶硅铝酸盐沸石和玻璃相的混合物制备出了介电陶瓷制品。该混合物还可以含有B2O3或SrTiO3之类的金属氧化物添加剂。在制成介电陶瓷制品时使用沸石的优点在于沸石制成的粉末对结晶陶瓷填料(例如氧化铝和堇青石)具有更高的反应性，这使得在烧结过程中能够更容易和完整地进行固态反应，并因此更容易生成所需的高Q相。其它优点包括制成的组合物均匀性的提高及相关的其电性能一致性的提高。
发明概要
本发明的一个实施方案是含1重量％至99重量％结晶硅铝酸盐沸石或由该沸石生成的无定形硅铝酸盐及50重量％至1重量％玻璃相的陶瓷制品前体，该结晶硅铝酸盐沸石在无水基础上具有如下经验式所示的组成：
A1/nSixAlOy
其中A是选自由碱金属、碱土金属、过渡金属、锌、稀土金属及其混合物组成的组的可交换阳离子，“n”是A的化合价而且值为1至3，“x”值为1至10，而“y”的值配平(A+Si+Al)化合价的总和。一种制备介电陶瓷制品的方法，包括将结晶硅铝酸盐沸石或由该沸石生成的无定形硅铝酸盐和玻璃相的混合物制成成形制品并将该成形制品在700℃至1000℃的温度下煅烧0.5至24小时，结晶硅铝酸盐沸石在无水基础上具有如下经验式所示的组成：
A1/nSixAlOy
其中A是选自由碱金属、碱土金属、过渡金属、锌、稀土金属及其混合物组成的组的可交换阳离子，“n”是A的化合价而且值为1至3，“x”值为1至10，而“y”的值配平(A+Si+Al)化合价的总和，其中沸石或无定形硅铝酸盐的存在量是1重量％至99重量％，玻璃相的存在量是50重量％至1重量％。
在对本发明进行详述以后，这些和其它目标及实施方案会更加清楚。
发明详述
如上所述，本发明涉及一种陶瓷制品前体和制备介电陶瓷制品的方法。本发明的一个要素是结晶硅铝酸盐沸石或由该沸石生成的无定形硅铝酸盐。沸石是公知的微孔三维骨架结构。一般来说，结晶沸石是由共角AlO2和SiO2四面体制成，而且特征在于含有尺寸一致的开孔，具有很大的离子交换容量，而且能够在不置换构成永久性晶体结构的任何原子的情况下可逆地解吸分散在整个内孔或晶体空隙中的吸附相。沸石在无水基础上可由下式表示：
A1/nSixAlOy
其中A是化合价为“n”的阳离子，“x”值为1至10。在天然形成的沸石中，A可以是Li、Na、Ca、K、Mg和Ba。A阳离子松散地结合在该结构上，而且经常可以通过传统的离子交换技术全部或部分被其它阳离子取代。因此，A选自由碱金属、碱土金属、过渡金属、稀土金属、锌和它们的混合物组成的组，因而“n”的值为1至3。最后，“y”的值配平(A+Si+Al)化合价的总和。优选地，A选自由镁、钙、锶、锌、钡和它们的混合物组成的组。
本发明中可用的沸石包括但不限于钙十字沸石、交沸石、水钙沸石、沸石B、沸石ZK-19、沸石W、沸石Y、沸石L、沸石LZ-210、沸石Ω、沸石LZ-202和它们的混合物。为了获得钙十字沸石类沸石，即钙十字沸石、交沸石、沸石B、沸石ZK-19和沸石W的结构相似性的详细解释以及可以从中找到这些沸石的特定结构信息的参考文献名单，读者可以参看US-A-4,344,851。该族沸石的重要特征是不存在下述骨架位点：或者可以不可逆地被钠或钾之类的阳离子占据，或被占据后有效地将其它位点与交换阳离子屏蔽开。沸石LZ-210是已经通过用含水氟硅酸铵(NH4)2SiF6处理提高了硅含量的沸石Y。US-A-4,503,023中描述了沸石LZ-210的制备和特征。沸石LZ-202是不使用模板剂而制备成的Ω-型沸石，在US-A-4,840,779中公开了其制备。在这些沸石中，沸石Y、L、B、W和Ω是优选的。
在下述说明中，使用沸石B作为举例说明本方法。然而，这无论如何也不应该被理解成是将本发明局限于沸石B。沸石B是一种化学式如下的合成沸石：
Na2O:Al2O3:xSiO2
其中“x”为2至5。US-A-3,008,803描述了沸石B的合成，主要需要制成铝酸钠(NaAlO2)、硅酸钠、氢氧化钠和胶态硅石的混合物并在自生压力下以60℃-150℃加热该混合物12至96小时。将制成的产物分离、清洗并干燥。反应剂的量可以不等，从而使SiO2/Al2O3的比率为2至5，优选为2.3至2.8，特别是在堇青石是最终玻璃-陶瓷的所需成分的情况下。在欧洲专利公开315,282中记载了另一种制备沸石B或沸石P的方法，其经此引用并入本文。
由于制成的陶瓷制品中钠离子的存在对所需的物理性能是有害的，因此必须最大程度地去除沸石中的钠阳离子。通常使用两种技术去除钠阳离子。一种技术是用例如镁或其它所需的阳离子进行多离子交换，而另一种方法包括用NH4 +之类的阳离子预交换沸石，然后用所需的离子进行离子交换。
通过使沸石与要被交换的阳离子的水溶液进行接触，可以方便地进行离子交换。例如制备硝酸镁(Mg(NO3)26H2O)的稀释(1摩尔)水溶液，并用氢氧化镁(Mg(OH)2)将溶液的pH值调节至7.5。制备的溶液的体积是提供完全离子交换沸石中的钠或其它碱金属所需的镁离子量的5至10倍的量。
硝酸镁溶液与沸石的接触可以方便地以分批处理法进行。相应地，将溶液与沸石粉末混合并将混合物回流大约2小时。接下来过滤混合物，由此分离出沸石粉末。用新一批的溶液重复进行该程序直至钠含量低于0.5重量％，优选低于0.2重量％。可以在仅重复六次该离子交换程序后得到上述钠含量。或者，可以采用该领域公知的方法(例如将沸石置于塔中并使镁溶液流经该塔或使用篮式离心机)使用连续处理过程进行镁交换。连续处理过程的优点是可以更有效地利用镁溶液。
本发明的另一基本部分是硅酸盐、硼硅酸盐或硼酸盐玻璃相。可用于制备玻璃相的玻璃粉末可含SiO2和/或B2O3；及Al2O3、MgO、CaO、Li2O、PbO、ZnO、SrO、BaO、K2O、Cs2O、TiO2、ZrO2、Nb2O5、Ta2O5、As2O5、Sb2O5、P2O5、GeO2、SnO2和Bi2O3中的一种或多种。这些玻璃粉末仅仅是作为例子而决不是为了限制本发明。通过本领域公知的方法，如US-A-4,714,687、5,164,342、6,232,251中所述的方法，制备这些玻璃相。该方法主要包括制备所需成分的均相混合物，将该混合物置于铂坩埚或耐火材料坩埚中并在1200℃至1650℃加热坩埚4至12小时。然后可将熔融物倒入模具获得板坯，倒入水中获得细粒，经过一组轧辊获得薄片，等等。
不管如何获得玻璃相，都可通过本领域公知的方法，例如球磨研磨，将其与所需沸石的粉末混合。混合物中的、以及因而在陶瓷制品前体中的沸石或无定形硅铝酸盐的量和玻璃相的量可以在很大范围内变动，但是沸石或无定形硅铝酸盐的量通常为从1重量％至99重量％，优选从5重量％至95重量％不等。玻璃相的量从50至1重量％，优选从50至5重量％不等。通常如下将所得混合物制成片材或带材之类的成形制品：首先使用本领域公知的方法，例如将粉末分散在溶剂中，制备该混合物的浆液，然后进行球磨研磨。制备浆液用的溶剂可以是水溶剂或有机溶剂，其中有机溶剂是优选的。有机溶剂包括但不限于甲苯、甲基乙基酮、乙醇、甲醇、二甲苯、丙酮和它们的混合物。
该浆液还可以非必要地含有一种或多种选自粘合剂、增塑剂和表面活性剂的成形助剂。粘合剂的非限制性例子包括聚乙烯醇、聚乙烯醇缩丁醛、聚氯乙烯、乙酸纤维素、硝化纤维素、甲基纤维素、乙基纤维素、羟乙基纤维素、羟丙基甲基纤维素、聚丙烯酸酯、聚甲基丙烯酸甲酯、聚甲基丙烯酸乙酯、聚乙烯、聚亚烷基二醇、石油树脂、环氧乙烷聚合物、聚碳酸异丙稀酯、聚四氟乙烯、聚α-甲基苯乙烯，等等。增塑剂的例子包括但不限于邻苯二甲酸正丁酯、邻苯二甲酸二辛酯、邻苯二甲酸丁苄酯、聚乙二醇、聚丙二醇、丙三醇、乙基甲苯磺酰胺、磷酸三正丁酯、硬脂酸丁酯，等等。表面活性剂(有时称作分散剂/抗絮凝剂)的例子包括但不限于聚异丁烯、亚油酸、油酸、柠檬酸、硬脂酸、羊毛脂脂肪酸、玉米油、红花油、三油酸甘油酯、二丁胺、取代的咪唑啉、磺酸酯、磷酸酯，等等。
如果存在成形剂，其在混合物中的、及制成的陶瓷制品前体中的总含量为从2至10重量％，优选从3至9重量％，最优选从4至9重量％不等。如果存在一种以上的成形剂，例如一种粘合剂和一种增塑剂，那么成形剂含量是粘合剂的量和增塑剂的量相加之和。
将所得混合物制成各种成形制品(取决于其粘性)。然而，如果用于介电应用领域，通常将其铸成带材或片材。这是通过使用刮片或本领域已知的其它工具将浆料涂敷到聚酯膜上完成的。带材的厚度可以在很大范围内变动，但是通常为50至500微米。尽管含膜的陶瓷前体可以在这时进行烧制，但通常首先将多张片材堆叠在一起。通常将图案化(patterned)导电层与孔连接器一起施用到各片材或层板上。孔连接器称作过孔(vias)，在层板中用于连接各层板的图案化导电层，以形成预定线路。接下来在700℃至1000℃下将层压制品(或任何其它成形制品)以足以制成陶瓷制品的时间烧结在一起。这通常为0.5小时至24小时。根据所用导电油墨的类型，烧结可以在空气中或在非氧化性气氛下进行。例如，对于银或金，烧结可以在空气中进行，而铜则要求非氧化性气氛。
尽管可以使用结晶态的沸石，但优选在将其与玻璃相混合之前对该沸石进行处理。在足以使沸石骨架结构崩塌但不足以开始烧结的温度下煅烧该沸石。例如，对于镁沸石B，该温度在600℃至825℃之间，优选为650℃至815℃。通过简单的实验或文献中提供的数据可以容易地确定任何沸石的“崩塌”温度的范围。该预先煅烧提供了可以在更大的温度范围内烧结而且烧结时具有较小收缩的无定形硅铝酸盐。
沸石/无定形硅铝酸盐和玻璃相的混合物还可以包含金属氧化物添加剂。金属氧化物添加剂包括但不限于B2O3、P2O5、TiO2、CaTiO3、Al2O3、SrTiO3、SiO2、BaTiO3、ZrO2、CeO2、SnO2、Nb2O5、Ta2O5、MoO3、WO3、V2O5、Sb2O5和它们的混合物。可以加入金属氧化物前体而不是上述一种或多种金属氧化物添加剂。可以加入的金属氧化物前体的种类是在加热时会生成金属氧化物的金属化合物。这些化合物可以是但不限于硝酸盐、碳酸盐、柠檬酸盐、乙酸盐、水合氧化物、氢氧化物等等，包括它们的混合物。金属可以是钛、锆、钙、锶、钡、镁、锌、铈、钒、铌、钼、锑、钽、锡等等。
金属氧化物添加剂的存在量可以有很宽的范围，但通常为1至20重量％，优选为2至15重量％，最优选为3至10重量％的金属氧化物。如果使用金属氧化物前体，所用量是可以产生1至20重量％、优选2至15重量％、最优选3至10重量％的金属氧化物。这些金属氧化物添加剂起到成核剂、烧结助剂和制成的陶瓷电性能改性剂的作用。
为了充分阐释本发明，列举下列实施例。应该理解的是，这些实施例仅仅用于举例说明，而不是为了对所附权利要求中陈述的本发明较宽范围进行不适当的限制。
实施例
使用几种玻璃制备介电陶瓷前体和介电陶瓷。玻璃相的组成见表1。
表1
玻璃相的组成(重量％)
| 编号# | SiO2 | B2O3 | BaO | SrO | CaO | MgO | ZnO | K2O | Al2O3 |
| 1 | 47.7 | 13.9 | 7.3 | 9.2 | 14.4 | 7.0 | 0.2 | ||
| 2 | 27.1 | 20.8 | 49.8 | ||||||
| 3 | 26.2 | 20.0 | 46.7 | 4.6 | 0.2 | ||||
| 4 | 51.5 | 13.7 | 7.1 | 9.8 | 11.1 | 3.7 | 0.2 |
如US-A-5,064,790所述制备镁沸石B，该专利通过引用全部并入本文。然后在750℃煅烧镁沸石B达2小时以提供无定形氧化物。
所有实验用的粘合剂都是聚乙烯醇(PVA)和聚亚烷基二醇(PEG)和水的混合物。粘合剂的组成如下：11.9重量％的PVA；8.0重量％的PEG和80.1重量％的H2O。如下制备粘合剂。在装有回流冷凝器的烧瓶中加入所需水的一半并将该水加热回流，此时边搅拌边加入PVA。一旦获得清澈的溶液(大约10分钟)，就逐滴加入所需量的PEG，然后加入剩余的水。最后，在搅拌的同时将混合物在95℃加热2小时，然后冷却至室温。
将煅烧过的MgB氧化物、玻璃和粘合剂混合，由此制备陶瓷前体丸片，然后以4000lbs/in2压制成圆形(1”直径，约0.125”厚)丸片。接下来将这些丸片以5℃/分钟加热至200℃，然后以10℃/分钟加热至700℃，最后以4℃/分钟加热至850℃或900℃，由此将这些丸片烧结。通过X射线衍射(XRD)分析制成的烧结丸片以检测结晶相。
制成的各种混合物的概况以及对最终陶瓷制品的分析结果见表2。材料栏表示无定形煅烧镁B沸石与所示玻璃的比例(单位：重量％)。下一栏是烧结温度，随后一栏是烧结陶瓷中存在的各相。烧结时间在900℃是4小时，在850℃是6小时。对两面都涂有银粉漆或两面都有真空镀金涂层的研磨抛光样品进行介电测量。下三栏包括在所示频率下测得的介电常数(k)，而最后三栏是在所示频率下测得的介电损耗(tanδ)。
表2
| 材料 | 烧结温度℃ | 相 | k | δ | ||||
| 1MHz | 100KHz | 10KHz | 1MHz | 100KHz | 10KHz | |||
| 70∶30煅烧MgB∶玻璃4 | 900 | 堇青石，钙长石 | 5.41 | 5.52 | 5.57 | 0.011 | 0.011 | 0.013 |
| 50∶50煅烧MgB∶玻璃2 | 900 | 钡长石 | 4.97 | 5.03 | 5.02 | 0.0046 | 0.0043 | 0.0059 |
| 70∶30煅烧MgB∶玻璃2 | 900 | 钡长石 | 5.88 | 5.96 | 5.92 | 0.0077 | 0.0056 | 0.0078 |
| 70∶30煅烧MgB∶玻璃3 | 850 | 钡长石 | 5.00 | 5.06 | 5.05 | 0.0061 | 0.0055 | 0.0087 |
| 70∶30煅烧MgB∶玻璃1 | 900 | 堇青石，钙长石 | 5.40 | 5.47 | 5.45 | 0.0072 | 0.0054 | 0.0067 |
| 50∶50煅烧MgB∶玻璃1 | 850 | 堇青石，钙长石 | 5.31 | 5.37 | 5.35 | 0.0058 | 0.0051 | 0.0061 |
| 95∶5煅烧MgB∶玻璃2 | 900 | 堇青石钡长石 | 6.12 | 6.21 | 6.20 | 0.008 | 0.007 | 0.011 |
| 98∶2煅烧MgB∶玻璃2 | 900 | 堇青石钡长石 | 6.19 | 6.31 | 6.37 | 0.011 | 0.012 | 0.022 |
Claims (16)
1.一种介电陶瓷制品前体，其含有1重量％至99重量％结晶硅铝酸盐沸石或由该沸石生成的无定形硅铝酸盐和50重量％至1重量％玻璃相，该沸石在无水基础上具有如下经验式所示的组成：
A1/nSixAlOy
其中A是选自由碱金属、碱土金属、过渡金属及其混合物组成的组的可交换阳离子，“n”是A的化合价而且值为1至3，“x”值为1至10，而“y”的值配平(A+Si+Al)的化合价的总和。
2.权利要求1的陶瓷制品前体，其中所述过渡金属是锌或稀土金属。
3.权利要求2的陶瓷制品前体，其中A选自由镁、钙、锶、锌、钡和它们的混合物组成的组。
4.权利要求1的陶瓷制品前体，其进一步含有选自由B2O3、P2O5、TiO2、CaTiO3、Al2O3、SrTiO3、SiO2、BaTiO3、ZrO2、CeO2、SnO2、Nb2O5、Ta2O5、MoO3、WO3、V2O5、Sb2O5及其混合物组成的组的金属氧化物添加剂。
5.权利要求3的陶瓷制品前体，其进一步含有选自由B2O3、P2O5、TiO2、CaTiO3、Al2O3、SrTiO3、SiO2、BaTiO3、ZrO2、CeO2、SnO2、Nb2O5、Ta2O5、MoO3、WO3、V2O5、Sb2O5及其混合物组成的组的金属氧化物添加剂。
6.权利要求4或5的陶瓷制品前体，其中金属氧化物添加剂的含量为1至20重量％。
7.权利要求1的陶瓷制品前体，其进一步含有金属氧化物前体添加剂，所述金属氧化物前体添加剂是选自由钛、锆、钙、锶、钡、镁、锌、铈、钒、铌、钼、锑、钽、锡及其混合物组成的组的金属的硝酸盐、碳酸盐、柠檬酸盐、乙酸盐、水合氧化物、氢氧化物及其混合物。
8.权利要求3的陶瓷制品前体，其进一步含有金属氧化物前体添加剂，所述金属氧化物前体添加剂是选自由钛、锆、钙、锶、钡、镁、锌、铈、钒、铌、钼、锑、钽、锡及其混合物组成的组的金属的硝酸盐、碳酸盐、柠檬酸盐、乙酸盐、水合氧化物、氢氧化物及其混合物。
9.权利要求7或8的陶瓷制品前体，其中金属氧化物前体的含量为可生成1至20重量％金属氧化物的量。
10.权利要求1-5以及7和8中任一项的陶瓷制品前体，其中沸石选自由钙十字沸石、交沸石、水钙沸石、沸石B、沸石ZK-19、沸石W、沸石Y、沸石L、沸石LZ-210、沸石Ω、沸石LZ-202和它们的混合物组成的组。11.权利要求6的陶瓷制品前体，其中沸石选自由钙十字沸石、交沸石、水钙沸石、沸石B、沸石ZK-19、沸石W、沸石Y、沸石L、沸石LZ-210、沸石Ω、沸石LZ-202和它们的混合物组成的组。
12.权利要求9的陶瓷制品前体，其中沸石选自由钙十字沸石、交沸石、水钙沸石、沸石B、沸石ZK-19、沸石W、沸石Y、沸石L、沸石LZ-210、沸石Ω、沸石LZ-202和它们的混合物组成的组。
13.权利要求1-5以及7和8中任一项的陶瓷制品前体，其特征还在于它含有选自由粘合剂、增塑剂、表面活性剂或其混合物组成的组的成形助剂。
14.权利要求11或12的陶瓷制品前体，其特征还在于它含有选自由粘合剂、增塑剂、表面活性剂或其混合物组成的组的成形助剂。
15.权利要求13的陶瓷制品前体，其中成形助剂的含量为2至10重量％。
16.权利要求14的陶瓷制品前体，其中成形助剂的含量为2至10重量％。
17.一种制备介电陶瓷制品的方法，包括将权利要求1-16中任一项的介电陶瓷制品前体制成成形制品，并在700℃至1000℃的温度下将该成形制品煅烧0.5至24小时。
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| KR100647307B1 (ko) * | 2004-12-23 | 2006-11-23 | 삼성에스디아이 주식회사 | 양성자 전도체와 이를 이용한 전기화학장치 |
| DE102010005704A1 (de) * | 2010-01-26 | 2011-07-28 | Süd-Chemie AG, 80333 | Verbesserter Katalysator auf Zeolithbasis zur Herstellung von Olefinen und zur Oligomerisierung von Olefinen |
| US9153356B2 (en) * | 2010-02-27 | 2015-10-06 | Empire Technology Development Llc | High dielectric permittivity materials from composites of low dimensional metallic systems |
| JP6728859B2 (ja) * | 2016-03-25 | 2020-07-22 | 日立金属株式会社 | セラミック基板およびその製造方法 |
| CN106215561B (zh) * | 2016-08-31 | 2018-04-20 | 苏州贝捷环保设备有限公司 | 一种燃煤烟气处理方法 |
| CN108314327B (zh) * | 2018-01-17 | 2020-12-11 | 贵研铂业股份有限公司 | Ce掺杂低温共烧陶瓷材料及其制备方法 |
| CN109020412A (zh) * | 2018-10-12 | 2018-12-18 | 蚌埠市方阵商品混凝土有限公司 | 一种高强度耐腐蚀混凝土 |
| CN111302763A (zh) * | 2020-04-09 | 2020-06-19 | 德化县宏顺陶瓷有限公司 | 一种如脂玉白陶瓷制品及其制备方法 |
| CN111533546B (zh) * | 2020-04-30 | 2022-03-11 | 山东国瓷功能材料股份有限公司 | 一种高频应用电介质材料及其制备方法 |
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- 2003-07-21 KR KR1020057002575A patent/KR20050046727A/ko not_active Application Discontinuation
- 2003-07-21 AU AU2003254054A patent/AU2003254054A1/en not_active Abandoned
- 2003-07-21 CN CNB038195135A patent/CN1323971C/zh not_active Expired - Fee Related
- 2003-07-21 WO PCT/US2003/022720 patent/WO2004016558A1/en active Application Filing
Non-Patent Citations (3)
| Title |
|---|
| 华南理工大学出版社 刘康明等，陶瓷工艺原理，第1卷 1990 * |
| 沸石陶瓷釉面砖 战頠，河北陶瓷，第28卷第4期 2000 * |
| 现代陶瓷工业中沸石的应用 范恩荣，山东陶瓷，第25卷第2期 2002 * |
Also Published As
| Publication number | Publication date |
|---|---|
| JP2005535553A (ja) | 2005-11-24 |
| KR20050046727A (ko) | 2005-05-18 |
| US20030224921A1 (en) | 2003-12-04 |
| EP1529020A1 (en) | 2005-05-11 |
| CN1675137A (zh) | 2005-09-28 |
| AU2003254054A1 (en) | 2004-03-03 |
| US6737374B2 (en) | 2004-05-18 |
| WO2004016558A1 (en) | 2004-02-26 |
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